3rd-INCC

18 Sept 2011, 08:00 → 23 Sept 2011, 18:00 Europe/Rome

Città del Mare, Terrasini - Palermo - Sicily - Italy

Flavia Groppi

The Congress serve as a forum of informal exchange of knowledge for scientists from different subject areas where the use, the production, the investigation or the measurements performed making use of radionuclides and nuclear radiation are contributing significantly to the technical progress.

Sunday 18 September

Reception

Opening Cerimony

Welcome Party

Monday 19 September

Session 1: Nuclear Chemistry and Radiochemistry

Radiochemistry

1 National and regional capacity building for medical radioisotope production: role of the IAEA

Progress in nuclear medicine has been always closely connected to the availability of a variety of radionuclides having both suitable decay characteristics and chemical properties to allow the development of useful diagnostic and therapeutic agents. Since there’s no ‘universal’ radionuclide capable to cover all clinical needs and imaging applications, nuclear medicine still relies on the supply of a number of radioisotopes having different roles and relative clinical importance. For instance, despite the current emphasis on PET, Tc-99m still remains a key radionuclide for nuclear imaging with SPECT, and the recent decline of reliability of the supply chain of the father nuclide Mo-99, due to unexpected and extended shutdowns at the few ageing research reactors and processing facilities, has caused serious problems and patient’s damage particularly in those countries placed at the outskirts of the radioisotope market. Similarly, the complexity of cyclotron-based technology required for the production of positron-emitting radionuclides like F-18 and C-11, has partially hampered and slowed down the growth and diffusion of diagnostic PET in those countries having a limited network of nuclear medicine centres. In this respect, the introduction of the Ge-68/Ga-68 transportable generator system has provided a new convenient option for the widespread application of a new class of PET radiopharmaceuticals. The need of novel radiolabelled agents appears particularly urgent in the field of radionuclide therapy. Although radioiodine therapy is a well-established protocol, this specialty can be still considered in its infancy mainly because of the difficulties supplying some relevant radioisotopes like Y-90 and Re-188. Recently, Lu-177 has attracted much interest due to the favourable nuclear properties and ease of production through conventional research reactors. Since lutetium shares common chemical properties with yttrium, the investigation of the clinical efficacy of analogous pairs of radiotherapeutic agents labelled with Y-90 and Lu-177 is currently an active field of research. It is also worth mentioning the rapid surge of interest in copper radiopharmaceuticals labelled with Cu-64 or Cu-67. The rich chemical behaviour of the element copper combined with the attractive nuclear characteristics of many radioisotopes has strongly stimulated the research for this new class of radiopharmaceuticals and some promising product is already in the pipeline. In order to promote the introduction in Member States (MS) of new diagnostic and therapeutic approaches based on the use of radiolabelled compounds, IAEA is deeply committed in the widespread development of national and regional capacity building of reliable sources of medical radionuclides. This objective is commonly pursued through the implementation of both national and regional projects and by promoting research investigations in the field of radiopharmaceuticals by means of Coordinated Research Projects involving a remarkable number of MS. All main topics and developments are currently covered by on-going and programmed projects including the most relevant and promising radionuclides cited above. To mention a few examples, IAEA is supporting (i) the search of alternative methods of production of Mo-99 and Tc-99m including accelerator-based technologies, (ii) the assessment of the clinical utility of antibody- and peptide-based Lu-177 radiopharmaceuticals, (iii) the optimization of the performance of the Ge-68/Ga-68 and Sr-90/Y-90 generator systems through the application of advanced separation methods, and (iv) the search of novel agents labelled with Cu-64 and Re-188.

Speaker: Adriano Duatti (International Atomic Energy Agency (IAEA))

2 Production of Medical Radionuclides in Russia: status and future

Production of isotopes for medical diagnostics and therapy is located in several institutions based on big nuclear facilities all over Russia earlier used for weapon and fundamental research, in particular: ● Research Institute Atomic Reactors (Dimitrovgrad): nuclear reactors, hot cells; ● Karpov Institute of Physical Chemistry (Obninsk branch): nuclear reactor, hot cells; ● Institute for Physics and Power Engineering (Obninsk): hot cells; ● CYCLOTRON Co. (Obninsk): cyclotrons, hot cells; ● Production Association MAYAK (Ozersk): nuclear reactors, hot cells; ● Kurchatov Institute (Moscow): solution reactor, cyclotron, hot cells; ● Khlopin Radium Institute (S-Petersburg): cyclotron, hot cells; ● Institute for Nuclear Research (Troitsk): linear accelerator. Most of isotopes are produced for export needs. Future growing of nuclear medicine in Russia is anticipated. New prospective developments are: production of fission 99Mo in Dimitrovgrad; production of 82Sr, 117mSn and 225Ac at INR together with IPPE providing basing on new effective target and radiochemical technology. Also very successful are developments of 68Ge/68Ga-generator at CYCLOTRON Co. and 82Sr/ 82Rb-generator at INR together with Central Research Institute of Roentgenology and Radiology (S-Petersburg) for PET-diagnostics. This progress will provide supplying a big fracture of medical isotopes in the world market, especially if new ambitious projects will be approved. Collaboration with North American and European companies and laboratories plays an important role.

Speaker: Boris Zhuikov (Institute for Nuclear Research of Russian Academy of Sciences)

Slides Sicily_2011-Zhuikov-3s.pdf

3 Development of a fast radiochemical method for the Tc-99m production by Neutron Activation and its cost analysis

The Tc99m is wide used in the world for SPECT diagnostic and its importance is great. In this scenario Italy isn’t different and the lack of production for this isotope suggest to investigate other way to achieve the needs satisfaction. Starting from well known production method by activation, the Laboratory of Nuclear Energy Applied (LENA) of the University of Pavia have developed the method using Mo Oxide enriched in 98 isotope as target. The results consider also the analysis of the production cost.

Speaker: Dr Andrea Salvini (Università di Pavia)

Slides Presentazione_LENA_Tc99m.pdf

4 Separation of no-carrier-added ruthenium from C-12 irradiated natural yttrium target by aqueous biphasic extraction

The mandate of green chemistry is to search newer methods, benign to the environment and Earth, in every sphere of chemical applications. The nuclear and radioanalytical chemistry is no way exception from this mandate. In this paper we present the development of a benign method for separation of 97Ru, a potential candidate radionuclide in the field of nuclear medicine from 12C induced Y target by aqueous biphasic extraction system (ABS). Unlike liquid liquid extraction ABS does not use environmentally harmful organic solvents and therefore considered as a benign approach in the field of separation sciences. In this paper we report the production of 97Ru by bombardment of 70 MeV 12C projectiles (with an average beam current of 90 nA) for 3 hours on a Y target. Two reaction channels, (i) natY(12C, 4n)97Rh(EC) 97Ru (ii) natY(12C, p3n)97Ru, contributed in the production of 97Ru. Assuring the production of 97Ru in the target matrix by $\gamma$-spectrometric studies, we dissolved the target in 0.1 M HCl, evaporated to dryness and finally redissolved in 0.01 M HCl. Four salts Na2SO4, Na2SO3, Na2CO3 (2 M each), NaOH (4 M) were used in combination with 50% PEG (Polyethylene glycol) in order to form various ABS. It has been found that ~ 60% extraction of 97Ru was possible in the PEG phase without contamination of bulk yttrium when 2 M Na2SO4 was used as salt rich phase. A high separation factor of 840 was achieved. The developed method is simple, fast and environment friendly.

Speaker: Dr Moumita Maiti (Saha Institute of Nuclear Physics)

5 Activation cross-sections for proton-induced reactions on natural Nd

Cross-section data on proton-induced reactions on natural neodymium are almost entirely missing. The data are of interest for testing predictivity of the nuclear reaction model codes, some of the activation products might have potential in nuclear medicine application, and last, but not least, rate of production of the longer-lived radionuclides is needed for estimating possible disturbing effects and increase of the background during neutrinoless double beta decay experiments like SNO+. We have, therefore, measured cross-sections for formation of 141Pm, 143Pm, 144Pm, 146Pm, 148Pm, 148mPm, 149Pm, 150Pm, 140Nd, 141Nd, 147Nd, 149Nd, 138mPr, 139Pr, 142Pr and 139Ce by 10–30 MeV protons. Several stacks of metal foil targets of natural isotopic abundance protected against oxidation were irradiated on the external proton beam of the cyclotron U-120M at the Nuclear Physics Institute at Řež. Special attention was paid to the excitation functions of the long-lived radionuclides. The measured data were compared with results of the TENDL code and the thick target yields for the relevant radionuclides were calculated.

Speaker: Dr Ondrej Lebeda (Nuclear Physics Institute AS CR, p.r.i.)

6 Evaporation residue cross section in 28Si+75As at Elab=6.6 MeV/nucleon

Study of reactions involving incomplete mass transfer has been an active area of investigation in heavy ion reactions at low and medium energies. Entrance channel parameters, namely, projectile energy and entrance channel mass asymmetry are important in governing the contribution from different types of reactions involving incomplete mass transfer such as quasi-elastic transfer, massive transfer or incomplete fusion and deep inelastic collisions. In addition, there may be contribution from fission like events. In the present work, cross sections of evaporation residues have been measured in 28Si+75As at Elab=183.7 MeV to investigate the contribution from these reactions. Experiments were carried out at Pelletron-LINAC facility at Tata Institute of Fundamental Research, Mumbai, India. Targets of 75As, prepared by vacuum evaporation on carbon backing, were bombarded by 28Si beam. Cross section of evaporation residues were measured by radio-chemical method based on recoil catcher technique followed by off-line gamma-ray spectrometry. Analysis of the gamma-ray spectra showed mainly the formation of evaporation residues with mass number A in the range AT to AT+AP, where AP and AT are mass numbers of projectile and target respectively, suggesting incomplete fusion to be the dominant non-compound process.Due to the contribution from incomplete fusion experimental cross-sections were higher than the calculated cross-section using PACE2 code, which is based upon statistical model. These studies did not show any significant contribution from deep inelastic collisions.In these studies significant contribution from fission was also observed. Different components were observed in recoil range distribution due to fission products and evaporation residues.

Speaker: Amit Kumar (Radiochemistry Division, Bhabha Atomic Research Centre)

Paper ID_71_Amit_Measurement_of_cross_sections_of_evaporation_residues_in_28S.doc ID_71_Amit_Measurement_of_cross_sections_of_evaporation_residues_in_28S.pdf

7 Investigation of the variance of fission product mass distribution in 20Ne + 232Th reaction

Fission of heavier actinides and trans-actinides through heavy ion reactions is currently an active area of study to investigate contribution from non compound nucleus fission. In addition, there is a contribution from transfer induced fission. In the present work, mass distributions of the fission products produced in 20Ne + 232Th have been measured at Elab=115 and 145 MeV. Self supporting targets of 232Th (thickness ~3 mg/cm2) were bombarded with 20Ne beam from variable energy cyclotron centre, Kolkata, India. The formation cross section of more than 30 fission products have been measured by recoil catcher technique followed by off-line -ray spectrometry. In order to determine the mass distributions, the cross section will be corrected for the charge distribution using appropriate charge distribution parameters for complete fusion fission and transfer induced fission. The variance of the experimental mass distribution resulting from complete fusion-fission of 20Ne + 232Th will be compared with the variance calculated using Random Neck Rupture Model (RNRM). Identification of fission products produced in transfer induced fission and complete fusion fission would also be helpful in the study of mass resolved angular distribution to investigate the contribution from non-compound nucleus fission.

Speaker: Suparna Sodaye (Bhabha Atomic Research Centre)

10:30 coffee break

Session 2: Nuclear Techniques: Fuel, Waste, Reactors IV

8 Molten salt reactor for waste transmutation: fuel cycles and recycle chemisty

Last decade, systems with liquid fuel on the base of molten salts attracted attention as potential dedicated burners of transuranium (TRU) elements from LWR spent fuel. Kurchatov Institute with partners contributed to Molten Salt Reactor (MSR) development within ISTC#1606 and #3749 tasks. Within these projects key technical solutions for development of promising TRU transmuter concepts were obtained. Studies included the following work packages: (1) fuel cycle, neutronics and thermal hydraulics analyses, including benchmarks on computing of safety parameters and transient analysis; (2) experimental verification of key physical & chemical properties for selected fuel salt compositions and (3) combined materials compatibility & salt chemistry control in selected molten salt environments at parameters simulating design operation. Within ISTC#1606 project the main attention was focused on theoretical and experimental evaluation of single stream MOlten Salt Actinide Recycler & Transmuter (MOSART) system. The optimum spectrum for Li,Be/F MOSART is intermediate/fast spectrum of homogeneous core without graphite moderator. Due to possibility of operation without additional neutron sources MOSART loaded only by TRU from spent nuclear fuel has high transmutation efficiency and can be loaded by the fuel with wide range of compositions. Unification of MOSART system with Th containing molten salt blanket, (the option is under study now within ISTC#3749), can provide its core operation with minor actinide (MA) bearing fuels basing on additional 233U support. In this case, when the core is processed, unburned actinides are returned to core along with 233U available from blanket. On the base of existing technologies within technological margins it is possible to burn any composition of used LWR fuel up to Pu/(Np+MA)=1.5 ratio. There is a way to get self-sustainable mode in the single-fluid LiF-BeF2-ThF4 core when it starts with carrier salt of lithium and beryllium fluorides fuelled by TRUF3 without any blanket. This fuel cycle scenario will require after system start up step by step increase of the thorium tetrafluoride in the fuel salt up to 6 mole %. The consideration done demonstrates the potential of the Li,Be,Th MSR without graphite moderator as the system with flexible configurations and fuel cycle scenarios which can operate with different loadings and make up based on TRU from used LWR fuel as special actinide burner, as self-sustainable system (CR=1) or even as a breeder (CR>1). In second part this paper is focused on chemical peculiarities of fuel recycle and fission product clean up for MOSART system without and with Th-U support.

Speakers: Dr Olga Feynberg (NRC "Kurchatov Institute"), Prof. Victor Ignatiev (NRC "Kurchatov Institute")

9 New separation methods for production of light stable isotopes for use in nuclear technology

Nuclear technology utilizes several stable nuclides, but not necessarily as isotopically pure materials. One example is boron, where B-10, abundance 19.9%, has a high thermal neutron absorption cross section utilized in neutron detectors, but natural boron is used despite the fact that the 80.1% abundant B-11 is not contributing. In Generation IV-reactor concepts fuels sustaining high temperatures are essential. One of the most interesting concepts is the Pebble Bed Modular Reactor where a small kernel of UO2 (or other fuel compound) is coated with ceramic materials. The fuel is called Triso (triply coated ceramic particle fuel) and is designed for being used for a long time and then disposed off. One of the coatings is SiC. In natural silicon a portion will transform to phosphorous during neutron bombardment. Phosphorous in SiC makes the material brittle and is undesirable. Removing the two heavier isotopes in Si makes the probability for getting (n,gamma)-reactions leading to P-31 unlikely. The challenge has therefore been to develop a low cost enrichment process for Si-28. The Norwegian company Isosilicon AS is devoted to this task and has developed a process based on the silicon gas silane, SiH4. The abundances of the silicon isotopes are 92.223, 4.685, and 3.092% for Si-28, Si-29, and Si-30, respectively. Thus, the challenge is to remove the two heavier isotopes. We initially developed a diffusion based process through a chromatography column packed with monodispersed polymer spheres. We achieved a separation factor between Si-28 and 30Si of 1.10 at a yield of 0.7%. The drawback of the method was too low throughput, and forming a collaboration with the French company Novasep SA an improved method was developed. In this process a column packed with a zeolite is used. The zeolite acts as an absorbent and when silane is passing through the column the heavier silicon isotopes are retained or exchanged with Si-28 on the column. Separation factors between Si-28 and Si-30 of 1.15 have been achieved, but at a smaller yield.

Speaker: Mr Dag Eriksen (Primus.inter.pares AS, Norway)

Paper ID_46_JRNC_3INCC_Eriksen_et_al_W-97.pdf

10 Computational electrochemo-fluid dynamics modeling in a uranium electrowinning cell

Metal electrowinning is the process of winning metal ions from an electrolyte to a solid form on a cathode by passing an electric current through the electrolyte. In the uranium electrowinning literature, only a limited number of multiphysics modeling studies have been taken place for the comprehensive understanding of the complexity in this process. A computational electrochemo-fluid dynamics model has been developed to describe the electrowinning separation behavior in an electrolyte stream through the planar electrode cell system. Multiple electrochemical reactions of uranium electrowinning process from a molten-salt electrolyte stream were modeled to illustrate the details of the flow-assisted mass transfer of ions to the cathode. The electrochemo-fluid dynamics that occurs in the electrolyte space between the planar electrode in uranium electrowinning cell were simulated using a computational fluid dynamics (CFD) platform. This model solves for the fluid phase of electrolyte using the Navier-Stokes equations in a CFD framework. The simulation includes the mass transport of the ionic species and associated electrochemical kinetics under laminar electrolyte flow condition. This approach was taken into account the concentration profile at the electrode surface, to represent the variation of the convective diffusion-limited current density as a function of the flow characteristics and of applied current density. It was able to predict conventional current-voltage relation in addition to details of electrolyte fluid dynamics and electrochemical variable, such as flow field, species concentrations, potential, and current density distributions throughout the cell driven by applying a constant current.

Speaker: Dr K. R. Kim (Korea Atomic Energy Research Institute)

Paper ID_120_Computational_Electrochemo-Fluid_Dynamics_Modeling_in_a_Uranium_Electrowinning_Cell.doc ID_120_Computational_Electrochemo-Fluid_Dynamics_Modeling_in_a_Uranium_Electrowinning_Cell.pdf

11 New bitopic molecules for Group Actinides Extraction

In the context of nuclear fuel reprocessing and in order to reduce the nuclear waste radiotoxicity, new ways to selectively extract actinides from spent fuels are studied. Among them the GANEX process (for Group ActiNides Extraction) is based on a homogenous recycling of actinides. All actinides (U(VI), Np(V et VI), Pu(IV), Am(III), Cm(III)), present in a highly acidic aqueous solution, would be extracted together and separated from fission products (especially from lanthanides) using liquid-liquid extraction. To develop this process, new extracting molecules which can efficiently separate actinides from fission products must be found. The CEA strategy is to synthesize bitopic ligands combining inside the same molecule a nitrogen ring allowing the An(III) / Ln(III) separation and an amide group allowing the extraction of other oxidation states of actinides. Considering previous results, nitrogen rings have been chosen from the 2,9-dipyridyl-1,10-phenanthroline and from the 2,4-dipyridyl-1,3,5-triazine family. Fourteen new bitopic ligands have thus been synthesized. Four of them (the lipophilic ones) have been tested as liquid- liquid extractants dissolved alone in the organic phase and the results show that ligands from the phenanthroline family are able to selectively extract actinides at different oxidation states from an aqueous solution 3M HNO3 with high distribution ratios and high separation factors toward Eu(III). Ligands from the triazine family are selective but distributions ratios are much lower. In order to better understand the driving force of the selectivity, thermodynamic studies have been carried out in MeOH-water solutions to determine stability constant for ten hydrophilic ligands. The results confirm the selectivity of ligands towards actinides(III) with respect to lanthanides(III) but also the effect of the structure on the complexation and the selectivity. The speciation (1:1 complexes) has been checked by different techniques like electrospray ionization mass spectrometry.

Speaker: Ms Julia Bisson (CEA-Marcoule, France)

12 Opportunity of using protective coatings for radioactive waste immobilization

One of the most important conditions for the realization of the concept of closed nuclear fuel cycle consists in the availability of highly developed infrastructure, including reprocessing of spent nuclear fuel (SNF), and further utilization of the resulted waste. The major way for increasing the safety of radwastes management is the development of advanced technologies, which would enable to reprocess the whole volume of high-level waste (HLW) and to obtain the solid products offering high chemical stability which would be suitable for long-term monitored storage and/or final disposal. At the same time another way to enhance the safety of solidified HLW storage and disposal is to apply a special coating on granulated wastes or to encapsulate solidified HLW using adequate materials. The main advantages of wastes reprocessing through the use of protective coatings are that this technique offers the possibility to immobilize the wastes in the form of solid products, which would be stable to leaching when contacting not only with water, but with other aggressive agents, for example, acids, as well. In the case of successful realization of R&D work package, which are being planned, the optimal parameters of the process ensuring an efficient localization of radioactive wastes will be selected, and the necessary recommendations for industrial use of developed technology will be generated. The object of this work was to conduct experimental study on technology development to obtain protective covering at ceramic materials containing different radionuclides. Physicochemical characteristics of these materials (data on cesium leaching rate) are presented. Another object of present work was the study on engineering solutions that could allow use "reactor" palladium for immobilization of long-lived radionuclides such as I-129 and TUE. In the paper the results of experiments on synthesis of cermets on palladium metal base (with metal oxides and palladium iodide inclusion) are presented. Obtained samples were examine by using of electronic-microscopy method. The data on leaching rate of europium and iodine from the samples with additional coverings are also presented.

Speaker: Dr Yury Pokhitonov (Khlopin Radium Institute)

13 Heterocyclic acids diamides as extractants for actinides extraction and separation

The treatment of the high level waste generated during nuclear fuel reprocessing is the obligatory stage of the nuclear fuel cycle. The reducing of volume of nuclear wastes could be realized by recovering of all harmful radionuclides (actinides, lanthanides and fission products) to separate fractions and their encapsulating in appropriate stable matrices. Separation of minor actinides (Am and Cm) from relatively harmless lanthanides is one of the most important and challenging problem due to their chemical similariry. On the one hand the most well-known extraction processes developed for actinide partitioning use neutral polydentate ligands solutions as a solvent, for instance CMPO (octyl(phenyl)-N,N-diisobutyl carbamoyl methylene phosphine oxide), TRPO (tri-n-alkyl phosphine oxide), diamides of malonic and diglycolic acids. All listed compounds possess very high affinity to f-elements and effectively extract them from nitric acid solutions but cannot separate the minor actinides from rare earth elements. The high complexing ability of these extractants is caused by presence in their structure of hard donor atoms (oxygens of ethers and carboxylic groups) that form strong complexes with both actinides and lanthanides. That is why “hard donor” ligands could be used only for simultaneous actinides and lanthanides recovery. On the other hand the most powerful agents for selective extraction or separation of trivalent actinides are nowadays “soft donor” compounds which possess several nitrogen or sulfur atoms. Some poly-nitrogen compounds extract americium many times better, than europium. However the main drawback of such ligands is that for some them the effective Am/Eu separation is possible only from solutions with low concentration of nitric acid (pH 2-4) and the others are not stable in nitric acid solutions. The combination of hard and soft donors in one structure allows effective extraction of actinides and their separation from lanthanides in the one stage. Two different classes of heterocyclic acids diamides (diamides of 2,6-pyridine dicarboxylic acid and diamides of 2,2’ dipyridyl-6,6’-dicarboxylic acid) were synthesized and systematically studied. Several extraction systems for extraction and selective separation of actinides (SF (Am/EU) up to 30) were developed and tested.

Speaker: Dr Mikhail Alyapyshev (Khlopin Radium Institute)

14 Processing of UV-Vis spectroscopy data by chemometric tools as a perspective way for online monitoring of SNF reprocessing

PUREX process of spent nuclear fuel (SNF) reprocessing requires thorough analytical monitoring at every technological stage to minimize economical losses and ecological risks. Spectrophotometric determination of various ions in visible and near UV spectral range is a classical analytical method. It can be successfully employed for determination of various oxidation states of actinides in solutions. However, when several actinides with significantly different concentrations are simultaneously present in the sample, classical spectral analysis of the minor components can become difficult or even impossible without preliminary chemical separation of the elements. UV-Vis spectroscopic analysis in combination with chemometric data processing seems to be promising for express and/or even online determination of various components in SNF reprocessing solutions. The use of modern optical fibers eliminates the limitations of the detector location and all control units of such a spectroscopic system can be placed in the clean zone. Moreover, one can simultaneously apply not only UV-Vis detectors, but also the detectors of IR and other types of radiation. In this study we attempted to evaluate the potential of UV-Vis spectroscopy in combination with simple chemometric data processing techniques for analysis of the mixture of several elements typical for SNF reprocessing. Spectroscopic measurements were performed with an AvaSpec spectrometer (Avantes B.V., Holland) in the range 184 – 1100 nm with 0.53 nm step. The concentrations of both Np and Pu were varied from 0.05 to 1.55 g/L in solutions with constant content of U (50 g/L) and HNO3 (2 mol/L). The experimental spectroscopic data were processed with the Unscrambler 9.7 (CAMO, Norway) software package using PLS1 algorithm. It was found that the prediction of plutonium content in the model mixtures is possible with rather small relative errors (in 9 of the 10 predicted samples the relative error was lower than 10%). Somewhat worse results were obtained for neptunium (in 8 of the 10 predicted samples RE is lower than 10%). The highest error for prediction of Np concentration was found for the mixture containing rather large concentrations of the elements in question (Np - 300 mg/L, Pu -1300 mg/L, and U50 - g/L). This result can be due to the noisy spectral signal of Np(V) at 980 nm obtained during the measurements that leads to the «noisy» latent variables responsible for Np concentration. However, the mean relative error for 10 test set samples is 4.4 and 7.1 % for plutonium and neptunium, respectively. The same spectral data were also subjected to the traditional univariate calibration procedure. Absorbance values at 980 nm were used for calibration against neptunium content, signal intensities at 475 nm, for plutonium. Linear fit of the experimental data points yielded regressions with R2 0.98 and 0.95 for plutonium and neptunium, respectively. In spite of the high correlation, predictive ability of these regressions was much poorer than those of PLS models and average relative error of prediction for 10 unknown test samples was 12,7 and 21% for plutonium and neptunium, respectively. Hence, feasibility of the optical spectroscopy in combination with chemometric data processing was demonstrated for the analysis of the model solutions simulating the PUREX SNF reprocessing. This approach allows fast and simple analysis of plutonium and neptunium in a wide concentration range in the presence of uranium. Further experimental studies are now in progress to improve these results with more complex model solutions as well as by use of more sophisticated chemometric techniques.

Speakers: Dr Dmitry Kirsanov (StPetersburg University), Dr Vasiliy Babain (Khlopin Radium Institute)

15 Neutron capture cross-section measurements of Th-232 using activation technique

232Th-233U fuel cycle in connection with ADSS is one of the possibilities for power generation besides transmutation of long-lived fission products and incineration of long-lived minor actinides. The 232Th-233U fuel in AHWR and ADSS has an advantage over the present reactors based on uranium fuel from the point of thousand times less radio toxic wastes production. Besides these, thorium in the earth’s crust is three to four times more abundant than uranium. Thus, it is a fact that 232Th is the only nucleus present in nature which can give rise to an excess of fissile material 233U in presence of either thermal or fast neutrons, and thus making it an excellent choice for nuclear reactors of the future. In the Th-U fuel cycle, the fissile nucleus 233U is generated by two successive β-decays after a neutron capture by the fertile nucleus 232Th. Thus, the production of fissile nucleus 233U depends on the 232Th(n,γ) reaction cross-section. The literature survey shows that there is no neutron capture cross-section data for 232Th beyond 2.73 MeV except only one data is available at 14. 5 MeV. In view of this, the 232Th(n,γ) reaction cross-section at average neutron energies of 6.2±0.3 MeV and 16.2±0.4 have been determined for the first time using activation and off-line γ-ray spectrometric technique. The average neutrons of energies 6.2±0.3 MeV and 16.2±0.3 MeV were produced by 7Li(p, n)7Be* reaction using BARC-TIFR Pelletron facility at TIFR, Mumbai. The experimentally determined 232Th(n,γ) reaction cross-sections were compared with the evaluated nuclear data of ENDF/B-VII, JENDL-4.0 and JEFF-3.1 and were found to be in good agreement. The 232Th(n,γ) reaction cross-sections were also calculated theoretically using the TALYS 1.2 computer code and compared with the experimentally determined data.

Speaker: Mr Paresh Prajapati (The M. S. University of Baroda, Vadodara, India-390002)

13:05 Lunch

Session 3: Radioanalytical Chemistry and Nanoparticles

16 Nanotoxicology research:a great opportunity for the radionanoanalytical chemist

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Speaker: Enrico Sabbioni (Veneto Nanotech)

17 Synthesis of molybdenum nanoparticle by in situ γ radiation

Nowadays molybdenum nanoparticle is highly demanding in industry. Molybdenum trioxide (MoO3), as a wide band gap n-type semiconductor, is one of the most intriguing transition metal oxides. There are various kinds of techniques for synthesis of molybdenum trioxide nanoparticle e.g. chemical route, sol-gel chemistry method, vapor deposition, electro-deposition, flash evaporation, ultrasonic irradiation, etc. In few cases external γ-radiation e.g. 60Co was employed for synthesis of molybdenum nanoparticle. However there are no reports on synthesis of molybdenum nanoparticle using in-situ minute amount of radioactive isotopes. Previously we have synthesised gold nanoparticle and gold-palladium bimetallic nanoparticle1, 2 with the help of minute amount (less than 1 μCi) 198Au (2.69d). In this work we report synthesis molybdenum trioxide nanoparticle with the help of minute amount of 99Mo (66h). In the mixture of ammonium molybdate (10-6M) and sodiumdodecyl sulphate (SDS) (0.5% w/v) we added 0.02 μCi 99Mo solution. The pHs (2 and 7) of the mixture solutions was then maintained by addition of dilute HCl and dilute ammonia solution as and when necessary. After cooling period of 30 days, 99Mo was completely decay out, and formation of MoO3 nanoparticles was checked by Transmission Electron Microscope (TEM), UV-vis, and Fluorescence spectroscopy. UV-vis absorption study showed that band between 200 to 390 nm with charge transfer in Mo-O bond. Molybdenum trioxide showed a strong emission peak at 432 nm and 428 nm at pH 7 and pH 2 respectively. TEM image revealed the presence of spherical (10-60 nm) size at pH 7 and nanowires of MoO3 nanoparticle of 2-10 nm width and length 0.5-4 μm at pH 2. The developed method is environmentally benign and found efficient to produce molybdenum trioxide nanoparticle. Reference: (1) Roy, K.; Lahiri, S. Gren. Chem. 2006, 8, 1063. (2) Roy, K.; Lahiri, S. Anal. Chem. 2008, 80, 7504

Speaker: Susanta Lahiri (Saha Institute of Nuclear Physics)

18 Radioanalytical methods: tools in studies of thyrotoxic effects of excessive bromide and perchlorate ions

With the aid of several radioanalytical methods, we studied the effects of an enhanced bromide and/or perchlorate intake on various aspects of iodine metabolism and, consequently, on the metabolism of thyroid hormones in the rat. Presumed goitrogenic and thyrotoxic effects of excessive bromide and perchlorate ions were followed in adult male rats, as well as in lactating rat dams (and their breast-fed pups), maintained on diets with different iodine content, ensuring either sufficient iodine supply or mild to severe iodine deficiency. The animals were administered subchronicaly (for 7 to 56 days) with bromide alone (in drinking water) or in combination with perchlorate. At the whole-organism level, we followed the influence of exogenous bromide on the uptake of [131I]-iodide by the thyroids and by various others organs and tissues (especially the mammary glands), as well as on the kinetics of elimination of iodine from the animal’s body. Bromide was applied in very low (ca. 0.2 mg) up to extremely high doses (> 200 mg bromide per animal per day). Especially, we followed the effects of high bromide levels in the organism of lactating rat dams on their performance in the course of nursing period and on the prosperity of their breast-fed pups. In rats administered with bromide and perchlorate we measured a consistent increase in relative weight of the thyroids with increasing time and concentration of applied bromide, and a sharp reduction of the 24-h uptake of [131I]-iodide by their thyroids. In these animals, we also determined (with radioimmunoassay using [125I]-thyroxine as radiotracer) a steady decline in serum total thyroxine concentration. Moreover, excessive bromide in the mothers substantially depressed the extent of [131I]-iodine transfer from the dams through mother’s milk to the suckling. As a consequence, a marked decline in the body weight increments of afflicted pups, in comparison with the young from mothers kept on a low bromide intake was observed. We have also confirmed the earlier observation that bromide toxicity is dependent on the state of iodine supply into the organism. Hypothyroidism in experimental animals caused by excessive bromide intake was more pronounced under the conditions of iodine deficiency (i.e., in animals maintained on a low-iodine diet). Very high bromide levels in the organism of the mothers adversely affected also the thyroids of their young. At the molecular level, we studied the effects of exogenous bromide and perchlorate ions on the activity of thyroid peroxidase (TPO), the key enzyme in thyroid hormones metabolism. Firstly, we found out correct assay conditions for the radiometric determination of TPO enzyme activity in isolated thyroid glands of iodine-deficient rats. Unexpectedly, we found that the influence of exogenous bromide on the TPO activity was not simply inhibitory; it was more complex, biphasic with regard to the extent of bromide intake. This work was supported by the Ministry of Education of the Czech Rep. (Research project No. MSM0021622413), by the Academy of Sciences of the Czech Rep. (Research project No. AV0Z50110509), and by the Czech Science Foundation (Grant No. 304/08/0256).

Speaker: Dr Stanislav Pavelka (Institute of Physiology, ASCR, Prague/Central-European Technology Institute, Masaryk University, Brno, Czech Republic)

15:30 coffee break

Session 4: Nuclear Chemistry and Radiochemistry

19 Assessment of actinides contamination in environmental and reactor structural samples by Accelerator Mass Spectrometry

Long lived anthropogenic alpha-emitting radionuclides have been, and stiil are, released in the environment by nuclear weapon tests, nuclear accidents, fuel reprocessing operations and nuclear power plants decommissioning. Among these the most significant are 239,240Pu and 236U. Quantification of releases and tracking their dispersion in the environment has traditionally been the task of alpha spectrometry (AS) or, more recently, of TIMS or ICP-MS. Even if these are mature methodologies, each of them has its own limitations, which are largely superseded by Accelerator Mass Spectrometry (AMS). It is well known that in Italy no Nuclear Power Plant (NPP) is in operation, but the four dismissed NPPs are now being decommissioned; moreover, the advancement of nuclear technologies has pushed our country to reconsider its energetic policy, planning for the future the installation of new generation NPPs. Both the operations of decommisssioning of the existing NPPs and the possible future operation of new plants demand accurate investigations about the possible contamination by radioactive releases of nuclear sites and neighboring territory and of structural materials of the reactors. The monitoring activity of surveillance institutions uses assessed radiometric techniques, but more and more ultrasensitive methodologies for the detection and quantification of ultralow activity radionuclides is requested at international level. Among these radionuclides the alfa-emitting isotopes of actinide elements are the most critical, because of their toxicity, not only radiological. The radiation counting methods, due to the long half lives, do not provide the necessary sensitivity (tipically of the order of 50 microBq) and, in some cases, resolution (e.g. 239Pu-240Pu). On the other hand, mass spectrometric techniques are potentially more sensitive than alpha counting, but suffer the problem of molecular interferences (e.g. 239Pu-238UH-208Pb31P). In the present paper we present the state of the art of a project aiming to establish an ultrasensitive methodology for the measurement of concentrations and isotopic abundances of U and Pu at the AMS facility CIRCE, and to exploit this technique for the characterization, from the point of view of the contamination by U and Pu, of both environmental samples from the Garigliano NPP site and samples representative of the structural materials of the building and of the reactor of the same plant, at present being decommissioned. Besides the characterization of the contamination of the site by ultralow level radionuclides, the new facility will provide a tool able to fulfill the analytical needs of IAEA for the campaigns for nuclear safeguards against illegal nuclear activities and the military use of weaponry with depleted uranium.

Speaker: Prof. Filippo Terrasi (2nd University of Naples)

20 Tritium measurements in water springs on Mt. Etna Volcano

Tritium exists rather uniformly in the environment as a result of both natural production by cosmic-ray interaction with the upper layers of the atmosphere and residual fallout from nuclear weapons tests carried out from 1952 till 1980. Naturally occurring tritium mainly reaches the Earth’s surface in the form of precipitation, becoming part of the hydrological cycle. Nowadays, the possibility of measuring the low level of tritium radioactivity gives a chance to use tritium as a natural tracer in the water systems. Surveys has been carried out on Mt. Etna and in the southern side of Nebrodi. The measurements have been carried out by liquid scintillation counting. The samples, collected in natural springs, were prepared according to the International Standard ISO 9698:1989. For each sample 250 mℓ of water were collected. For each one about 250 mg of sodium thiosulfate anhydrous (Na2S2O3) to convert iodine into iodide, and about 500 mg of sodium carbonate anhydrous (Na2CO3) to make the sample alkaline, and some glass beads were added to prevent bumping. Afterwards, the samples were distilled by means of an apparatus consisting of a round bottom flask of capacity 500 mℓ, a Vigreux distillation column, an adapter (bent type) and a condenser. After discarding the first 50-75 mℓ of distillate, about 100 mℓ were collected in polyethylene bottles. With this procedure there was no significant isotopic fractionation in the distillation. The investigated areas show extremely low tritium concentrations, much below the Italian limit of 100 Bq/ℓ for drinking water and even comparable with the minimum detectable activity value. The effective dose due to tritium consumption is also calculated.

Speaker: Dr Roberto Catalano (Dipartimento di Fisica e Astronomia -Università degli studi di Catania,INFN sezione di Catania)

Paper

• ID_174_3rd_INCC-Catalano.docx
• ID_174_3rd_INCC-Catalano.pdf
• ID_174_3rd_INCC-Tables_Catalano
• ID_174_3rd_INCC-Tables_Catalano.pdf

21 Determination of the isotopic ratio U-236/U-238 in environmental samples

Determination of the isotopic ratio 236U/238U in environmental samples M. Srncik1, P.Steier2, R. Eigl1, G. Wallner1 1 Department of Inorganic Chemistry, University of Vienna, Währingerstr. 42, A-1090 Vienna, Austria 2 Faculty of Physics – Isotope Research, University of Vienna, Währingerstr. 17, A-1090 Vienna, Austria 236U with a half-life of 2.3∙107 years is produced via thermal neutron capture on 235U. Natural production results from different neutron sources like from (α,n) reactions on lighter nuclides, spontaneous fission of 238U, induced fission of 235U and at the Earth surface from the cosmic rays. Only small amounts are produced naturally from uranium in ores, soils and rocks but a huge amount is produced in nuclear power plants. Naturally 236U occurs in ultra trace concentration in the environment, therefore it is a big challenge to determine a natural isotopic ratio of 236U/238U in environmental samples which is expected to be in the order of 10-14 to 10-13. For the analysis of this isotopic ratio, water samples from rivers and creeks were collected in the alpine region of Austria, from the Danube, the Black Sea and the Atlantic. From surrounding areas also soil samples were investigated. After a pre-concentration and an anion exchange step the uranium fraction was co-precipitated with NdF3 and thin sources were prepared for α-spectrometry to determine the activity ratio of 234U/238U and the chemical yield. Afterwards these filters were reprocessed for the analysis of the isotopic ratio 236U/238U by AMS (Accelerator Mass Spectrometry). The special aim was the characterization of the 236U/238U ratio in natural waters and soils, and to investigate the contribution from anthropogenic sources.

Speaker: Gabriele Wallner (University of Vienna)

Poster Section 1

22 A sequential procedure for determing Pu-238, Pu-(239+240), Am-241, Sr-90 activities in human bones obtained from joint replacement surgery

This poster presents results of application of a sequential radiochemical procedure for multi-elemental analyses for samples human bones obtained from joint replacement surgery. The grounded ashes of bones were dissolved in 6mol/L HCl. Samples were left for two days until bubbles disappeared. The tracers, i.e. 242Pu, 243Am and 85Sr, were added using an automatic pipette and analytical balance to determine the mass of the tracer solutions added. After complete dissolution two subsequent precipitation of calcium oxalates was completed to obtain two fractions: 1) transuranic (Pu+Am) and 2) strontium at pH 3 and 6, respectively.The pH was adjusted using ammonia. The centrifuged transuranic fraction was re-dissolved and oxalates were precipitated again at pH=3. It was performed to remove traces of phosphates which may cause problems during the anion-exchange procedure on Dowex-1 resin. In both fractions the oxalates were destroyed with hot concentrated nitric acid. The solutions were evaporated to dryness. Each transuranic fraction was dissolved in 100 mL of 1 mol/L HNO3. The oxidation state of Pu was adjusted to +4 using hydrazine and NaNO2 and after filtration and conversion into 8 mol/L HNO3, the fractions were passed through Dowex-1x8 (100-200 mesh). Am passes the column without retention. Th which together with Pu remains in the column, was eluted with 12 mol/L HCl and then Pu was eluted using 50 mL of 0.1 mol/L HF-0.1 mol/L HCl. Effluents containing Am ions were evaporated nearly to dryness, then diluted and next Am was co-precipitated with Fe(OH)3 at pH=9 adjusted using ammonia. Each centrifuged residue was dissolved in 4 mol/L HNO3 and passed through conditioned TEVA column (by Triskem International) to remove traces of Th. Am was separated from any traces of rare-earth elements using methanol-acid solutions. Both Pu and Am sources were made using NdF3 method and were measured using alpha spectrometer with Canberra PIPS detectors. Each Sr fraction was dissolved in 100 mL of 3 mol/L HNO3, filtrated and then directly passed through the conditioned Sr-Resin (by Triskem International) column. After washing the column with 20 mL of 3 mol/L HNO3, strontium was eluted using 30 mL of deionized water, evaporated and purified from traces of 210Pb. The purified Sr solutions of 3 mL of 0.5 mol/L HNO3 were transferred into a LSC vials and following determination of 85Sr recovery by means of gamma-spectrometry, they were stored for at least 2 weeks to achieve equilibration between 90Sr and 90Y. Finally, each of the solutions was mixed with 10 mL of HiSafe3 liquid scintillation cocktail and measured using Wallac 1414 Guardian LSC spectrometer. The radiochemical procedure described above was developed over more than 10 years, and we profited much from the experience we gained while completing many projects on Pu, Am and Sr determination in animal bones Due to world-wide shortage of animal bones reference materials (RM) in many of our projects, the soil matrix RMs were applied instead. However, the RM by NIST SRM Ash Bone 4356 have been recently certified for Pu isotopes and 90Sr. This material, as well as IAEA soil-375, were thus analyzed to assure the measurements quality.

Speaker: Mrs Ewa Tomankiewicz (Institute of Nuclear Physics, PAS, Radzikowskiego 152,31-342 Kraków, Poland)

23 Aging effects on kinetic properties in palladium–tritium system during tritium storage

Palladium powders had been aged at room temperature for 6.6 years. The 3He content was estimated from the initial tritium stoichiometry and the aging time by applying the radioactive decay law, which shows the helium-palladium atomic ratio (He/Pd) is 0.204. Tritium absorption of aged palladium powder has been measured in the initial pressure of 284 kPa and as a comparation, fresh palladium powder (He/Pd = 0) has been also tested in the initial pressure of 354 kPa at the same temperature of 20℃. The correspondence and difference on the kinetics of tritium absorption are analyzed between the aged and fresh palladium powder because of the presence of helium. The overall tritium absorption process is determined by two steps: (1) the chemisorption reaction on the surface of palladium tritide at the beginning of absorption; (2) diffusion of tritium atoms through tritide in the middle of tritium absorption. There is a better agreement on kinetic properties for fresh palladium powder than aged one. The absorption pressure-time isotherms and other ones show that the presence of helium in the palladium decreases the absorption rate of tritium by influencing the initial absorption process (<5s). The maximum of the tritium absorption rate of aged palladium powder exists in the α area and the absorption rate does not change so largely as the fresh palladium powder.

Speakers: Mr Jie Du (China Academy of Engineering and Physics), Mr Zhi Zhang (China Academy of Engineering and Physics)

24 Application of the CL resin to the separation and determination of Cl-36 and I-129 in environmental and decommissioning samples

The monitoring of long-lived radionuclides is of great importance for the surveillance of nuclear facilities such as power plants, waste repositories and reprocessing plants, during their operation as well as during their decommissioning. This is especially true for radionuclides of rather volatile elements such as chlorine and iodine, main interest being in Cl-36 and I-129. Measurement techniques frequently employed for the analysis of these radionuclides like e.g. liquid scintillation counting, require a thorough and selective sample preparation in order to give accurate results. Sample preparation methods employed are often elaborate and time consuming. An extraction chromatographic resin that allows extraction, and subsequent separation, of Cl-36 and I-129- from pretreated environmental and decommissioning samples was developed and characterized to overcome these issues and facilitate Cl-36 and I-129 analysis. Some results of the resin, characterization including weight distribution values (Dw values) of various cations and of Cl- and I- on Ag+ loaded CL resin, are presented. Several methods for the separation and determination of Cl-36 and I-129 have been developed based on determined resin characteristics and tested on spiked real samples. The results of these tests will be presented.

Speaker: Dr Aude Bombard (TrisKem International - FRANCE)

25 Baseline background radiation dose and risk assessment study due to natural radionuclides in the edible biota of Domiasiat, Meghalaya

A radiation dose and risk assessment exercise was carried out for the edible biota, Garra lamta, Brassica compestris var. dichotoma, Oryza sativa var.Shalum1 and Zea mays due to the naturally available radionuclide 40K, 238U and 232Th in Domiasiat ecosystem of Meghalaya, India. A detailed morph-physiological study of biota and the eco-geo-physiographical study of ecosystem had been carried out prior to the dose -risk assessment. The activity in biota and the corresponding soil and water sample was measured for the 12 months by precipitation method using NaI detector. The total activity of water was 0.3447 Bql-1 by the precipitation method using the 34.2% detector limit and 3000 second counting time having detection limit of 0.03 Bql-1.The foremost point source dose distribution (source↔target) method and the recently developed FASSET were investigated in details. Garra lamta was modeled using the former method whilst others uses FASSET and was concluded that deviation amongst two was negligible. The obtained transfer factor (TF) was Oryza spp. (1.00E-01- 40K, 8.76E-05- 232Th, and 9.11E-05- 238U), for Brassica spp. (5.39E-01- 40K, 8.17E-04 232Th and 2.96E-04 238U) and for Zea spp. (3.41E-01-40K, 5.84E-05-232Th and 8.87E-05-238U) of each radionuclide respectively. The obtained total dose was 1.58E-04 in Oryza spp., 2.87E-04 in Brassica spp. and 6.90E-03μGyh-1 in Zea spp. and in Garra lamta 0.0199μGyh-1 finally compared with IAEA and UNSCEAR dataset for the screening level dose for the fish (0.022-0.065) ,flora (0.1-1.0 mGyd-1) of fresh water and forest ecosystem respectively. Zea spp. was found comparatively more susceptible for chronic radiation exposure.

Speaker: Kumar Niranjan (North-Eastern HilL University Shillong Meghalaya)

26 Chemical composition of urban soils in the vicinity of steel industry

Contamination of soil due to human activities has become a serious concern to both environment and public health. The Piracicaba city, in the state of São Paulo, Brazil, is a highly industrialized area with a large concentration of steel industries. The fumes, liquid and solid waste generated by these industries may contain chemical elements that cause environmental and health problems. In the past decades, due to the absence of environmental regulations and high costs of treatment and disposal of residues, some companies deposited huge amounts of solid waste within the urban area of Piracicaba. In this context, this work focuses on the determination of chemical elements in soils collected in the vicinity of steel industries by instrumental neutron activation analysis (INAA) to evaluate the influence of such solid waste deposits on the soil composition. Soil samples were taken at 3 depths in 21 sampling points, covering an area of about 80 km². As, Ba, Br, Ce, Co, Cr, Cs, Eu, Fe, K, La, Na, Nd, Rb, Sc, Sm, Ta, Tb, Th, Yb and Zn could be determined in the samples. Among such elements, As and Cr should be emphasized for presenting high concentrations in various sampling points, with several values exceeding the warning limits established by the environmental legislation of São Paulo State (15 mg/kg for As and 75 mg/kg for Cr).

Speaker: Prof. Elisabete De Nadai Fernandes (University of Sao Paulo)

27 Classification of igneous rocks from Paraguay by INAA

Plutonic and volcanic rocks were analyzed by INAA in their major components for its classification. The samples proceed from the sites/regions corresponding to the Precambrian to Paleozoic/Postpaleozoic magmatism in the Eastern and Western Paraguay. In the Eastern Region the Precambrian is present in two structural hights: the Apa Hight in the north and Caapucu in the south.The latter is constituted by Rio Tebicuary complex; of upper Proterozoic age. In the Western Region, Precambrian outcrops ocurred in the north in the Alto Paraguay Province. Six main magmatic events constitute the Paleozoic/Postpaleozoic magmatism: the eldest one (Alto Paraguay Province) is dated at Permo-Triassic.The second is dated as Cretaceous at the north of Eastern Parguay. The third one also Cretaceous, is exposed by extended lava of tholeiitic basalts of the Alto Paraná Formation/Serra Geral . The fourth event,occurred in the Asunción-Sapucai Graben.The fifth, in the Misiones Province near San Juan Bautista mainly by sodic-alkaline plugs and dykes . The sixth, from the Paleocene, is concentrated in the Asunción region. The activation were performed in an annular 25Ci Am-Be neutron source. The analysed elements were Si, Al, Na and K and thus the SiO₂, Al₂O₃, Na₂O and K₂O content determined. The reactions used were i) ²⁸Si (n.p) ²⁸Al; ii) ²⁷Al (n,p) ²⁷Mg iii) ²³Na (n, γ ) ²⁴Na; the fourth element of interest, potassium, was analysed by simple gamma spectrometry. The procedure overall uncertainties were checked as per the irradiation of three compositae samples of SiO₂+ Al₂O₃ + NaHCO₃+ K₂CO₃ prepared as standards in convenient proportions. The determination of these parameters permit the classification of the rocks in the categories acid, intermediate, basic and ultrabasic, as well as the identification of the rock family and in certain cases the norm and their magmatic provenance.

Speaker: Prof. Juan F Facetti-Masulli (Universidad Nacional de Asunción)

Paper ID_100_CLASSIFICATION_OF_IGNEOUS_ROCKS(2).pdf ID_100_CLASSIFICATION__OF_IGNEOUS_ROCKS_OF_PARAGUAY_BY_INNA(2).doc

28 Comparison of composition of lechatelierites in moldavites and silica phytoliths

Formation of moldavites (tektites from Central Europe) was connected with a large meteorite impact to Ries region in western Bavaria in Germany 14.5 million years ago. The parent materials for moldavites have usually been assigned to the uppermost layer of pre-impact sediments and sedimentary rocks dated to Middle Miocene. According to several geochemical indicators, ash from biomass burned at the early stage of the impact may have contributed to the parent materials. Moldavites contain in the glass matrix small inclusions of pure silica – lechatelierites. To evidence the possible biogenic component in moldavites, composition of lechatelierites separated from moldavites has been compared with composition of silica phytoliths extracted from barley (Hordeum vulgare L.) – a representative of a Poaceae (grass) plant family. Silica phytoliths are biogenic opal objects formed by solidification of dissolved forms of silicon by some higher plants. They are, after plant's death and decay, preserved in soil and sediments. The samples of lechatelierites and barley silica phytoliths were analysed by instrumental neutron activation analysis (INAA) in the short and long time irradiation modes. Both types of materials consist mainly of silica, but many other elements are present in minor and trace quantities. Despite several differences, the overall elemental pattern observed in phytoliths for both major and trace elements is similar to that observed in lechatelierites, especially the high K/Na ratios. This study has been supported by the Czech Science Foundation grant 205/09/0991.

Speaker: Jan Kameník (Nuclear Physics Institute ASCR)

29 Deep purification of uranium extract from technetium

Uranium purification from technetium in the process of spent nuclear fuel reprocessing is one of the most complex problems. Uranium reclaim for separating plant is to be extremely decontaminated from Tc because of the problems at the sublimation stage caused by volatile TcF6 formation during uranium recycling process. There is a conflict between Thorp plant requirements for uranium product after the second extraction cycle (Tc content 4 mg/kg U) and ASTM С787-03 standard, which requires Tc content in uranium hexafluoride less than 0.5 mg/kg U and in some cases the level of uranium decontamination from Tc in this product should be less than 1.6 mkg/kg U. This conflict could be resolved by uranium reclaim additional radiochemical reprocessing for supplying purified product to the sublimation plant. It is evident that such technology makes reprocessing process rather expensive. The aim of the research work was to find and work out such a process, that can provide effective and not expensive deep uranium purification from Tc on the basis of extraction spent fuel reprocessing technology. The solution of mentioned problem is an extraction-chromatographic purification of uranium extract by usage of aqueous reducing agents solution as a purifying stream. These agents reduce Tc(VII) to nonextractable Tc(IV). The process of purifying is carried out in cyclically-countercurrent feed mode of purified and purifying streams in a column filled with porous excipient (charged with aqueous purifying stream). It is shown that depending on composition of the aqueous phase concentration factor varies from 40 and above. These conditions provide practically complete treatment of uranium extract.

Speaker: Mr Vitaly Vidanov (Open Joint Stock Company “Academician A.A. Bochvar High-Tech Research Institute of Inorganic Materials”)

30 Design and construction of an equipment for the radiochemistry process of molecules marked for the sector health

In the Plant of Radioisótopes Production of the Nuclear Center of México (ININ) of Mexico, they are prepared weekly radiofármacos, the Yodohipurato of sodium and the Meta-yodobencilguanidina. These compounds are so called molecules marked with iodine (131I). Nowadays the processes radioquímicos that are used for the preparation of these compounds are carried out of individual and manual form, in a box of gloves, in spite of it, present risks of radiological safety. To improve these disadvantages, this work, there presents an equipment who is inside a warm cell in order to minimize the risks of radiological safety, the equipment works of semi-automated form in order which one appears a minimal exhibition to the radiation of direct form, for the responsible personnel of marking molecules.The routine industrial production with this equipment, began with the preparation of 9 Yodohipurato of sodium doses of sodium of 2.73 mCi of iodine each one in flasks with saline solution of 4.5 ml and the product that was containing the molecule marked with 0.5 ml, a percentage was obtained of marked with 95.6 %. The innovation of this work, it consists of presenting a new design of an equipment, where two radichemistry processes are carried out of marked molecules, composed of mechanical, electrical systems and air system.

Speaker: Dr Alanis José (Nuclear Center of México)

Paper ID_64_Alanis-México.doc ID_64_Alanis-México.pdf

31 Development of an original radiochemical protocol in a view of Sn-121m and Sn-126 measurements in Low and Intermediate Level Nuclear Wastes

The LANIE (Elemental, Isotopic and Nuclear Analysis Laboratory) develops and implements a set of radiochemical protocols associated with radiological and elemental measurement techniques devoted to the characterization of Long Lived Radionuclides in Low and Intermediate Level Nuclear Wastes. 121mSn and 126Sn are two radionuclides of interest for the performance assessment of waste storage or disposal. Both isotopes are produced from the fission of 235U occurring in nuclear reactors, with thermal fission yields estimated to be about 0.00003% and 0.06% respectively. 121mSn can also be produced by activation of tin present as a minor additive in zircaloys, inconels and steels used in the nuclear industry. Due to their half-lives (55 and 250000 years for 121mSn and 126Sn respectively [1,2]), the National Radioactive Waste Management Agency (ANDRA, France) requests their monitoring in waste packages before their disposal in specific sites. Due to their low activities in nuclear wastes, 121mSn and 126Sn need a thorough chemical separation before any measurement can be performed. The radiochemical protocol was first developed on various synthetic solutions to separate tin from the matrices and concentrate it prior to any nuclear or mass spectrometry measurements. The protocol starts with a microwave digestion or alkaline fusion with the addition of a natural tin carrier and a 113Sn radioactive spiker. The following steps are constituted of ion exchange separations combined with co-precipitations and a highly selective ethylation step. The final purified fractions thus obtained are suitable for X spectrometry analysis of 121mSn and Q-ICPMS measurements of 126Sn. The protocol yield is evaluated by gamma measurement of 113Sn. The protocol was then optimized to be applicable to various sample types. As no 121mSn or 126Sn sources are commercially available, the protocol was first applied to zircaloys and spent nuclear fuel dissolution solutions to obtain in-house standards. The radiochemical procedure was validated subsequently on ion exchange resins spiked with 113Sn, 121mSn and 126Sn. Afterward, it was completed for the analyses of radioactive sludges and activated steels. This procedure enables to achieve high decontamination factors and to eliminate specifically all isobaric interferences (126Te, 110Pd16O, 110Cd16O) for 126Sn analysis by Q-ICPMS. The overall separation yields obtained range from 45% up to 70%. References: [1] S.A. Catlow et al., “Half-life measurement of 126Sn isolated from Hanford nuclear defense waste”, Journal of Radioanalytical and Nuclear chemistry, vol 236, no3, p599-603, 2005. [2] P. Bienvenu et al., “Determination of 126Sn half-life from ICP-MS and gamma spectrometry measurements”, Radiochimica Acta, vol 97, no 12, p687-694, 2009.

Speaker: Dr Celine Gautier (CEA Saclay DEN/DANS/DPC/SECR/LANIE)

32 EDXRF determination of heavy metals in the soil of an urban plot in Mexico City

A project to develop a residential building in a previous industrial plot, in the urban zone of Mexico City, has required the application of the local Norm regarding the maximum permitted limits of heavy metals in soils. Though the Norm prescribes the Atomic Absorption method for the heavy metals determination, the Energy Dispersive X-Ray Fluorescence method was proposed for a quick and preliminary quantitative survey of the probable polluted areas. Samples were taken at 0.5 and 3.5 meters depth with a manual drilling equipment (Hand-Auger-AMS), dried and grinded. The spectra was obtained in a Si-Li detector (Princeton-GT-S30), operated to 450/900 , with a 30 mCi Pu-238 source and 3000 s of irradiation time. The polluted area reaches to one tenth of the total. The contaminants to be reduced or eliminated are: Cu, Zn, Pb and specially Cr whose concentration is several times higher than permitted. A background determination in the total area is being performed for a better precision of results, since the soil is a mixture of limestone and sand. A commentary is included related to other countries criteria (USA, Canada and The Netherlands) on this topic

Speaker: Prof. Juan Lartigue (National University of Mexico)

33 Elemental characterization of bread and durum wheat by INAA

Cereals are the most significant agricultural crops not only by the sheer magnitude of their gross-tonnage production and prevalence in human diets worldwide, but also as food vehicles of important items for human nutrition and wellness at large -- proteins, dietary fibres and oligoelements, such as selenium, calcium, zinc and iron, to name just a few. Still, some micronutrients feature an uneven distribution in the upper continental crust, and thus in cultivation soils deriving therefrom. Whether soils have always been poor in an essential element, or have just become deprived of it by intensive farming, the result is the same: insufficient soil-plant transfer, feeble-to-nonexistent plant uptake, and, therefore, unsatisfactory dietary distribution of that element through the food chain. Countries that implemented corrective programs of crop biofortification and consumer education have been successful in dealing with some micronutrients' deficiencies. Given their relative weight in Portuguese diets, cereals are obvious candidates for crop-supplementation strategies that may contribute to an upgrade in the health status of the whole population. A good knowledge of element-baseline data for major cereal varieties (plants) and main production areas (soils) is a pre-requisite though. The present work was aimed at an elemental characterization of cereals and soils from relevant wheat-producing areas of mainland Portugal. This paper is focused on wheat samples -- bread and durum wheats; Triticum aestivum L. and Triticum durum Desf., respectively -- from the 2009 campaign, collected at Alto and Baixo Alentejo (inland regions). Elemental concentrations were determined by instrumental neutron activation analysis (INAA; k0-variant), and assessed with the k0-IAEA software. Quality control of the procedure was asserted through the analysis of NIST-SRM 1568a (Rice Flour), NIST-SRM 1572 (Citrus Leaves) and GBW 07404 (Limy-yellow Soil). Results are discussed and compared to available data from abroad.

Speaker: Dr Maria do Carmo Freitas (URSN-ITN, Instituto Tecnológico e Nuclear)

Paper ID_181_Galinha_Paper.doc ID_181_Galinha_Paper.pdf

Poster Galinha_118_Poster.pdf

34 Evaluation of cobalt bis(dicarbollide) ion derivatives with attached metal chelating groups for their use in nuclear waste treatment

High liquid level waste (HLLW) issued from reprocessing of spent nuclear fuel contains dangerous nuclides, especially minor actinides (241,243Am, 245Cm, 237Np) responsible for long-term radiotoxicity of the waste. In the last decades, several HLLW partitioning processes for actinides separations based on the use of different extractants such as octyl(phenyl)-N,N-di-iso-butyl-carbamoylmethylphosphine oxide (CMPO) – TRUEX process, trialkylphosphine oxide – TRPO process, diisodecylphosphoric acid – DIDPA process, substituted malonamides – DIAMEX process, and N,N,N′,N′-tetraoctyl diglycolamide – TODGA process have been developed. Over the last several years, the new families of extractants based on covalent bonding of hydrophobic cobalt bis(dicarbolides) [(1,2-C2B9H11)2-3-Co)]- anion (COSAN) to different metal chelating ligands (e.g. derivates of CMPO -, TODGA -, phenantroline -, organophosphorous - groups) were tested for separation of trivalent actinides from acidic waste solutions. Particularly two compounds from these series deserved further attention: (i) N,N-di-n-octyl-TODGA-COSAN containing two COSANs covalently bound to nitrogen atoms of diglycolic acid diamide platform via diethyleneglycol connectors (along with n-octyl as the second substituents on the amide nitrogen) and (ii) extractant N-terc.-octyl-CMPO-COSAN based on bounding of COSAN to CMPO group (with terc.-octyl on the amidic nitrogen atom and diphenyl substituents on phosphine end), also with use of the long chain diethyleneglycol connector. These extractants have proven very efficient, and have been thus evaluated in more details for the separation of actinides and lanthanides in the nuclear treatment. As we demonstrate, these derivatives enabled good separation of trivalent actinides and lanthanides from bulk of fission products present in the model PUREX feed. Undesirable co-extraction of some fission products, such as Mo, Zr, Pd could be suppressed by addition of oxalic acid and (hydroxyethyl)diaminetriacetic acid (HEDTA) into the feed and scrubbing solutions. Trivalent actinides and lanthanides can be effectively stripped from loaded organic phase by salts of citric acid and diethylenetriamine pentaacetic acid (DTPA). However, no selective separation of actinides from lanthanides either during extraction or during stripping with complexants has been obtained using these extractants. Therefore, several different DTPA-sodium nitrate solutions with or without buffers have been tested as an option for the selective actinides stripping. The results will be presented.

Speaker: Dr Maria Bubenikova (Nuclear Research Institute Rez plc.)

Poster Bubenikovaetc.pdf

35 Fukushima fallout at Milano, Italy

Radionuclides from Fukushima fallout were first detected at Milano region in a rain water sample, collected during March 27-28, with the concentrations of 131I and 137Cs isotopes in the rainwater to be equal with 0.89 Bq L-1 and 0.12 Bq L-1, respectively. During the same days a snowfall sample was collected from Monte Rosa mountain at a height of 3000 m, with the concentrations of 131I and 137Cs in snowfall to be lower than that in rainwater sample. A sample of dry deposition that was collected 9 days after the rainfall event of 27-28 March, 2011 showed that the dry deposition of 131I and 137Cs was 0.40 Bq m-2 and 0.24 Bq m-2 respectively. The concentrations of 131I in sheep and cow milk samples collected on 30 March, 2011 from a farm at Macugnaga, Monte Rosa mountain, were 0.30 Bq L-1 and 0.37 Bq L-1 respectively. Daily monitoring of the airborne activity levels was carried out with a high volume air sampler and Glass Fiber filters as the collection substrate. Increased atmospheric radioactivity was detected on air filter taken on 30 March 2011, wile the maximum activity of 467 µBq m-3, occurred at April 3-4, 2011. A week later the activities had fallen to about 50% of peak values, with a general decreasing trend over the following days. In the time period of one month after the nuclear accident, concentrations of 137Cs and 134Cs in air as high as 88 µBq m-3 and 78 µBq m-3, respectively were recorded. According to the measurements, airborne activity levels remains of no concern for public health in Italy.

Speaker: Prof. ALEXANDRA IOANNIDOU (Aristotle University of Thessaloniki, Physics Department, Nuclear Phys. and Elementary Partcile Phys. Division)

Paper NEW_Milano_Greece_Fukushima_sent_10_01_2013__Corrected_submitted_2_with_Fig.docx NEW_Milano_Greece_Fukushima_sent_10_01_2013__Corrected_submitted_2_with_Fig.pdf

Slides Shanghai_2011_FUKUSHIMA_PAROUSIASI.pdf

36 Implementation of the k0-standardization method for analysis of geological samples at the Neutron Activation Analysis Laboratory, São Paulo, Brazil

The Neutron Activation Analysis Laboratory (LAN-IPEN) has been analysing geological samples for many years with INAA comparative method, for geochemical and environmental studies. This study presents the results obtained in the implementation of the k0 standardization method at LAN–IPEN, for geological samples analysis, by using the program k0-IAEA, provided by The International Atomic Energy Agency (IAEA). The efficiency curve of the gamma-ray spectrometer used was determined by measuring calibrated radioactive sources at the commonly used counting geometries. The thermal to epi-thermal flux ratio f and the shape factor alfa of the epi-thermal flux distribution of the IEA-R1 nuclear reactor of IPEN were determined for the pneumatic irradiation facility and some selected irradiation positions, for short and long irradiation, respectively. To obtain these factors, the “bare triple-monitor” method with 197Au-96Zr-94Zr was used. The Certified Nuclear Reference Material IRMM-530R Al-0,1% Au alloy, high purity zirconium, Ni and Lu comparators were irradiated. In order to validate the methodology, the geological reference materials basalts JB-1 (GSJ) and BE-N (IWG-GIT), andesite AGV-1 (USGS), granite GS-N (IWG-GIT), SOIL-7 (IAEA) and sediment Buffalo River Sediment (NIST–BRS-8704), which represent different geological matrices, were analysed. The concentration results obtained agreed with certified, reference and recommended values, with relative errors less than 10% for most elements. These results indicate excellent possibilities of using this parametric method at the LAN-IPEN for geochemical and environmental studies.

Speaker: Dr Ana Maria Figueiredo (IPEN-CNEN/SP)

Paper ID_50_Davi_paper_Palermo_5.doc ID_50_Davi_paper_Palermo_5.pdf

Poster poster_Davi_final_[Modo_de_Compatibilidade]1.pdf

37 In soil radon measurements to characterize fault systems

In soil radon measurements are often a tool used to investigate geophysical events. The radon exhalation depends on several parameters, the most important ones are the meteorological variables (temperature, humidity, atmospheric pressure, wind velocity and rain) and soil characteristics (porosity, permeability, ..). Areas in which fault systems insist, are characterized by specific profiles of emission of radon gas owing to the presence of visible or not visible faults in the soil with a defined spatial orientation. To study the behavior of in soil radon along a fault, we investigated as first a well known fault: the Pernicana one. Three different methodologies were used to measure Radon. The first technique consisted in Solid State Nuclear Track Detectors, CR-39 type, and allowed integrated measurements. The second one consisted in a portable device for short time measurements. The last consisted in a continuous measurement device for long time monitoring, placed in selected sites. Two different soil gas horizontal profiles were investigated across the fault. The results obtained with the three methodologies are in general in agreement with each other and reflect the tectonic settings of the investigated area. The lowest Radon values were recorded just on the fault plane, and relatively higher values were recorded a few tens of meters from the fault axis on both of its sides. Comparing the methodology we can affirm that, spot measurements are useful for the quick recognition of high emission sites, to be later monitored for Radon variations in time. SSNTD measurements allow for the time monitoring of a relatively large number of sites, although they lose detail on the short-term changes due to their long integration time. Continuous monitoring probes are optimal for detailed time monitoring, but they are expensive and can thus be used to complete the information acquired with SSNTD in a network of monitored sites.

Speaker: Dr Gabriella Mangano (Dipartimeno di Fisica e Astronomia Università di Catania, CSFNSM)

38 Limiting transport properties of lanthanide and actinide ions in water.Hydration number and hydrolysis phenomena.

Abstract We start with the idea that there is no second layer of hydration for trivalent ions La, Ac; Since it is an illogical model that first layer may contains between eight and nine molecules of water, and second layer would have a larger radius and no more than five or closes six water molecules. In this paper, we present a new simplistic model for estimation of trivalent actinides and lanthanides ions self diffusion coefficients. We take account hydrolysis phenomena. We use Fuoss theory and Bjerrum approach to calculate Kh the thermodynamic hydrolysis constant using Marcus summarized data for different radius. We suppose that ion structure stills the same in solid state (salt) or in aqueous solution, regarding the water molecules surrounding central ions (M≡ La3+ , Ac3+). Taking account hydrolysis, experimental self diffusion coefficient D of ion is equal to the sum of two contributions: free and associated ion. D° = αD°free + (1-α)D°h , free ≡ M3+(H20)n=8,9 , h ≡ M3+(H20)nOH- with Kh = [h].[H+] /[free]= 10-7 (1-α)/α ; α is the molar fraction of free La/Ac ions. At infinite dilution, pH = 7 (Oswald dilution Principle) In our recent paper, we have verified our simplistic calculus method with experimental data for Lanthanum and Gadolinium (first and middle 4f element series). Our model will end the disconcordances results by Spectral and crystallographic methods in solid state or by measurement methods solution... Key worlds: Lanthanides , actinides , hydrolysis , hydration shell.

Speaker: Prof. Habib Latrous (Faculté des sciences de tunis)

39 Low-level gamma spectroscopy measurements of air samples in Austria after the Fukushima accident

Following the earthquake and tsunami in Japan on 11 March 2011 and the resulting damages at the nuclear power plants in Fukushima, environmental samples were taken in Austria to determine the effects in Middle Europe, about 10 000 km away from Fukushima. Of course, the radiation-level in Austria resulting from this accident is very low, but can be measured with low-level gamma spectroscopy. In this paper air samples are analyzed to show which fission products can be verified and to calculate the concentration of their activities. The series of measurements started 2 weeks after the accident and were stopped 3 weeks later. The measurements yielded primarily I-131 and, occasionally, Cs-134 and Cs-137. A total of 15 samples were analyzed to demonstrate a time variation of air contamination. The maximum activity was observed on 29 March. Finally the results were compared with measurements of other European countries.

Speaker: Dr Andreas Musilek (Vienna University of Technology - Atominstitut)

Poster Poster_ID_60_Sizilien.pdf

40 Lu-177g produced with high specific activity by deuteron irradiation for metabolic radiotherapy

Lu-177g is a low energy negatron emitter that, thanks to its favourable decay properties (t(1/2) = 6.734 d, negatron emission 100 %, E(β,max) = 489.3 keV, <Eβ> = 163 keV, Eγ = 208.4 keV), is one of the most promising radionuclide to be used in nuclear medicine, especially in metabolic radiotherapy of cancer of small dimensions. This RN is mainly produced in thermal nuclear reactor in two different ways: the first in carrier added (CA) form by (n,γ) reaction on enriched target of Lu-176 leading to a lower specific activity (AS), compared with the theoretical carrier free value AS(CF) = 4.05 GBq•μg^-1, the second in no carrier added (NCA) form by (n,γ) reaction on enriched target of Yb-176 followed by negatron decay leading, after selective separation of Lu from Yb, to a higher AS. This latter case shows no evidence of production of the long-lived impurity Lu-177m. An alternative method is to produce Lu-177 by the deuteron activation of natural or enriched in 176Yb targets. In this case, the routes of interest are the indirect reaction Yb-176(d,p)Yb-177 that decays by negatron emission to Lu-177g and the direct reaction Yb-176(d,n)Lu-177(g+m). In order to optimize the Lu-177g production the thin target yields (ttys) of the nuclear reactions involved were measured as a function of the projectiles energy by the stacked-foil technique irradiating Yb targets of natural composition at the MC40 cyclotron of the JRC, Ispra, Italy, that can deliver deuterons with energies up to 19 MeV. The measurements, done at the radiochemistry laboratory of LASA by high resolution gamma spectrometry (HPGe detectors), were started few hours from the EOB (end of bombardment) and were carried on for many months, till more than one year, after the irradiation. The excitation functions of all radionuclides produced were measured and compared with the data, if present, published in the unique previous literature publication. It was determined the decay curve of Yb-177 and the growth curve of the cumulative (direct and indirect) production of Lu-177g. The analysis of these curves conduct to the evidence that the predominant route for the production of Lu-177g is the indirect reaction Yb-176(d,p)Yb-177, that decays to Lu-177g. The direct reaction Yb-176(d,n)Lu-177(g+m) is observable only above 13 MeV and contributes for only 4% of the total in correspondence of 14.6 MeV. In the spectra acquired one year from the EOB the γ lines of Lu-177m are not presented. By detection limit method the activity of Lu-177m at the EOB is been evaluated, in the worst case, less than 0.07% of total activity of Lu-177. The production of Lu-117g by deuteron irradiation of Yb targets will be competitive with neutron activation. The deuteron activation for 12 hours of a thick target of Yb-176 (100% enriched) with E(in) = 12.5 MeV, ΔE = 10.0 MeV, I = 100 μA can produce up to 10 GBq of cumulative Lu-177g.

Speaker: Simone Manenti (LASA, Università degli Studi di Milano and INFN-Milano)

Abstract 152_Manenti.doc

Poster Poster_Lutezio_3rd_INCC.pdf Poster_Lutezio_3rd_INCC.pptx (Protected)

41 Metallographic and XPS analyses of deposits from steam generator

The presented work examines the samples of deposits from steam generators. These samples were collected at the nuclear power plant. The deposits were studied by metallographic methods and methods of image analysis by programme NIS-Elements AR 3.0. The layers were characterized by three distinctive areas: homogeneous part (in contact with the wall tubes), porous central part and broken part (growth into the area. XPS method was used to determine the composition of deposits.

Speaker: Ms Jana Petrů (ICT Prague)

Poster Petru.pdf

42 Natural radionuclides and Cs-137 in marine sediments from open and semi-enclosed gulfs, lagoons and fjord-like environments in Greece

In this paper the 238U, 232Th, 226Ra, 40K and 137Cs activity concentrations in the marine sediments of Patras, Corinth and Amvrakikos Gulfs and Messolonghi lagoon complex, and their possible relation to geological, geochemical, biological and anthropogenic factors and processes are presented. Patras Gulf is an open gulf with maximum depth of 160 m and due to its vicinity to Patras city (200.000 citizens) and harbour is contaminated with respect to port and urban activities. The Gulf of Corinth is a semi enclosed deep basin (max. depth 860m) which is connected to the Ionian Sea through the Patras Gulf. An aluminum processing plant discharges bauxitic red mud tailings into the northern margin and the central basin of the Gulf. The Amvrakikos Gulf is a semi-enclosed shallow (max. depth 65m) gulf which is connected to the Ionian Sea through narrow straits. Two major rivers discharge million of m3 freshwater into the Gulf. The Gulf is considered as the only fjord-like environment in Mediterranean Sea and is seasonally hypoxic/anoxic. Moreover, the Gulf has been heavily affected by the input of phosphate fertilizers over the last 25 years. The Messolonghi-Aetoliko lagoon complex, located in the northern coast of the Patras Gulf, is the most extended lagoon system in Greece and is considered as the most important wetland area. The highest measured 238U, 232Th and 226Ra content was detected in the Gulf of Corinth due to the submarine bauxitic red mud deposits. Elevated 238U activity concentrations were observed in the Amvrakikos Gulf as a consequence of the pollution of the Gulf by the U-rich phosphate fertilizers. The highest activity concentrations of 137Cs were found in the Messolonghi lagoon and the Amvrakikos Gulf. These high activities are resulted of the runoff from the drainage areas at the northern margin of the Patras and Amvrakikos Gulfs, which have been heavily contaminated by 137Cs. Furthermore, the regional distributions of natural and man-made radionuclides interpreted on the basis of the geological, biogeochemical and anthropogenic factors of the surveyed areas.

Speaker: Prof. Helen Papaefthymiou (University of Patras)

43 Natural radionuclides, stable elements concentration and study of bioactive components of Peperomia pellucida

In recent decades, there has been a great advancement in research in developing drugs from plants. Nevertheless, little information exists in literature about the activity concentration of U-238 and Th-232 decay products, even as stable elements concentration in plants used for this purpose. Peperomia pellucida, whose popular name in Brazil is little heart, is a plant known by its medicinal properties like healing property, analgesic activity, antibacterial activity and antifungal activity against food fungi. The objective of these determinations is to understand the possible relationship existing between elementary concentrations and pharmacological action. Elemental concentration for the elements As, Ba, Br, Ce, Cl, Co, Cr, Cs, Eu, Fe, Hf, K, La, Lu, Mg, Mn, Na, Nd, Rb, Sb, Sc, Se, Sm, Ta, Tb, Th, U, V, Yb and Zn were determined by Instrumental Neutron Activation Analysis in the aerial parts, leaves, and roots of Peperomia pellucida, in the extracts and infusion and in the surrounding soil. The samples were irradiated at the Nuclear Reactor IEA-R1, IPEN-SP, together with the reference materials Soil-7 and Buffalo River Sediment and the method validation was performed with the reference material Lichen (IAEA-336). The concentration of Cd, Cu, Ni, Pb and Hg was determined by Graphite Furnace Atomic Absorption Spectrometry and the activities of Ra-226, Ra-228 and Pb-210 was carried out by total alpha and beta counting with radiochemical separation. The essential oil, ethanolic and hexane extracts of Peperomia pellucida were tested for antifungal activity against Aspergillus flavus in vitro on Petri plates. The antifungal activity was based on the inhibition zone and minimal inhibition concentration values against the pathogen on Petri plates assays. It was also determined the essential oil chemical composition by CG-MS.

Speakers: Mr Fabio Vitorio SUSSA (Instituto de Pesquisas Energéticas e Nucleares - IPEN), Dr Paulo Sergio Cardoso SILVA (Insituto de Pesquisas Energéticas e Nucleares - IPEN)

Poster Sussa,_F.V.pdf

44 Neutron and photon activation analyses of anomalous phonolites from Lusatian Mountains in Bohemian Massif, Czech Republic

The studied phonolites from the Lusatian Mountains in northern part of the Czech Republic are tertiary, highly evolved alkaline volcanic rocks associated with continental interplate magmatism with anomalous contents of incompatible and volatile components. From the geochemical point of view, these rocks are residue of parent magma concentrating many incompatible and volatile elements. Phonolites solidified at relatively low temperature similarly to other residue liquids, and thus during ascent of magma towards the Earth surface such rocks consolidated in shallow depths (less than one kilometer) in the upper bed. Therefore, phonolites can be classified among the so-called subvolcanic (or hypabyssal) rocks. The studied anomalous phonolites are strongly depleted by compatible elements as Mg, V, Cr, Fe, Ni, Sr, whereas contents of Al, alkaline elements Na, K, Rb, and incompatible elements such as Zr, Nb, REE, Hf, Ta, Th, U reach extremely high values. Contents of halogens (F and Cl) are also very high. For a detailed geochemical study, various modes of nondestructive neutron (including the epithermal and fast neutron mode) and photon activation analyses were utilized. Combination of these modes allowed assaying major elements as well as most trace elements (48 elements in total). The study has been aimed at elucidation of source materials and processes leading to formation of these anomalous phonolites (partial melting and contamination by crust materials). Potential host accesory minerals for some abundant elements such as F (up to 1800 ppm, possibly hainite or apatite), Cl (up to 5700 ppm, possibly sodalite), Zr and Hf (up to 3000 ppm Zr, possibly zircon or hainite), Nb (up to 900 ppm), and rare earth elements (up to 700 ppm for their sum, possibly apatite or perovskite) have been suggested. This study has been supported by the project IAA300130902 of the Grant Agency of the Academy of Sciences of the Czech Republic.

Speaker: Dr Zdeněk Řanda (Nuclear Physics Institute ASCR)

Poster 156_Randa-poster.pdf 156_Randa-poster.ppt

45 Passive biomonitoring study for trace elements in oysters Crassostrea brasiliana (Lamarck, 1819: Mollusca, Bivalvia) in São Paulo State coastal sites, Brazil (25º00’-23º56’S, 47º25’-45º19’W)

Estuaries and coastal zones frequently receive a great number of contaminants from anthropic sources, resulting in degradation of these ecosystems as a whole. Trace elements present in estuarine water and in marine sediments may accumulate in many invertebrate marine species as bivalve mollusks such as oysters and mussels. This study aimed to determine trace elements in Crassostrea brasiliana oysters, very abundant in the estuaries of the State of São Paulo, Brazil, from three sites in São Paulo State coast: Cananéia Estuary (reference site), Bertioga and Santos Estuarine Systems (impacted by industrial and urban activities in moderate and heavy levels, respectively). Passive biomonitoring was carried out, in which the organisms were collected from their natural environment and analyzed. Seasonally, ninety individuals of Crassostrea brasiliana were collected in each site between September/08 and July/09. After sample collection and preparation, the elements As, Co, Cr, Fe, Se and Zn were determined by Instrumental Neutron Activation Analysis (INAA) and Cd, Pb and Hg were determined by Atomic Absorption Spectrometry (AAS). For analytical quality control, the NIST Standard Reference Material 1566b “Oyster Tissue” was analyzed. Statistical tests were applied to study the bioaccumulation of these trace elements and their seasonal variations.

Speakers: Dr Eduinetty Sousa (Instituto Oceanográfico da Universidade de São Paulo), Dr Marilia Semmler (Instituto de Pesquisas Energeticas e Nucleares), Dr Marina Vasconcellos (Instituto de Pesquisas Energeticas e Nucleares)

Poster 3rdINCC-Catharino_Final.pdf

46 Physico-chemical investigation of heterogeneous equilibria in the saturated aqueous solutions of uranylsilicates of the alkaline elements

Solubilities of uranylsilicates of general formula МIHSiUO6nH2O (MI – Li+, Na+, K+, Rb+, Cs+, NH4+) in aqueous solutions at 25С were investigated. Based on the obtained data constants of equilibrium of the dilution’s reactions of uranylsilicates in acidic and neutral solutions and standard Gibbs’s functions of formation of studied compounds were calculated, the composition of equilibrium solutions was investigated. Physico-chemical description of the equilibrium heterogeneous systems based on thermodynamics laws included set of equilibria established in the systems was proposed. To develop this description it was taken into account that heterogeneous process of dilution in the studied systems was established and homogeneous equilibria where silicon (IV) and uranium (VI) were presented as set of ion and molecular forms, were established, too. Prediction of behavior of given compounds in different conditions was made based upon proposed description of the heterogeneous system state like “solid uranylsilicate – aqueous solution”. Solubility of uranylsilicates of alkaline elements and ammonium quite depends on pH. In acidious solutions their concentration is at the level of 10-3 M and in the neutral ones it decreases to 10-6 M. Type of alkaline element does not have significant influence on solubility of the compounds. Data for compounds in the range pH 3-6 was used to calculate values of solubility products (SP) of the low soluble compounds. At first values of SP decrease in the raw of Li+ - NH4+ - Na+ - K+, then increases again from K+ to Cs+. Modeling of the heterogeneous system state showed that solubility of uranium compounds as function of pH has minimum at pH 11.5, that corresponds to optimal conditions for synthesis of uranylsilicates of alkaline elements.

Speaker: Ms Natalya Godovanova (Nizhni Novgorod state University)

47 Plutonium, americium and radiocesium in coastal sediments of the Cuban island, in the Caribbean Sea

In this study we report levels of plutonium, americium and radiocesium in sediments from coastal sites of the Cuban island (Caribbean Sea), a region from where there is very limited environmental information concerning anthropogenic radioactive pollution. One sediment core from the Havana Bay (HB) and two from the Batabano Gulf (BG), both sites located in the western part of Cuba, were collected for this study. The activity concentrations, vertical distributions and inventories of 239,240Pu, 238Pu, 241Pu, 241Am and 137Cs were determined in order to get insights on the sediment deposition processes. The activity ratios of 238Pu/239,240Pu, 241Am/239,240Pu and 241Pu/239,240Pu indicated that atmospheric nuclear weapon tests fallout is the main source of the anthropogenic radionuclides in this tropical region. The present study further confirmed earlier observations of low levels of 137Cs in coastal sediments in the Cuban island region. 239,240Pu, contrary to 137Cs, accumulated in the sediments with inventories two to four times higher than the expected fallout inventory in the Cuban region. The high fluxes of 239,240Pu indicate that sediment focusing occurs in the investigated sites. The measurements of anthropogenic radionuclides in coastal sediments provided good estimates of past and present radioactive contamination in the Cuban marine environment.

Speaker: Dr José Antonio Corcho Alvarado (Centro de Estudios Ambientales de Cienfuegos (CEAC), Cienfuegos, Cuba)

48 Potassium concentrations and annual effective dose of the most customary-consumed foodstuffs in Mexico as a cultural heritage

Measurement of radionuclides concentration in foodstuffs allows to assessing the dose being caused by its intake. It means at least one-eight of the mean annual effective dose due to natural sources. Additionally, among the trace elements in foodstuff, K is one of the most important, it is a well-known essential element and it occurs all over the earth. Three of the most customary-consumed foodstuffs in Mexico as a cultural heritage since pre-Hispanic time to the present (in all economic classes): bean, chili and corn mel (to cook “tortillas”) were analyzed by γ spectrometry in order to determine 40K activity, the derived annual effective dose, and the potassium concentration. Results show that mean activity of 40K, annual effective dose and % of potassium concentration are as follow: for chili 901±86 Bq kg-1, 37.2 micro-Sievert per year and 2.84±0.27%; for beans, 510±10 Bq kg-1, 27.5 micro-Sievert per year and 1.60±0.04%; for corn meal, “masa”, 90 Bq kg-1, 58.1 micro-Sievert per year and 0.27.±0.089%. The total effective dose intake from these typical foodstuffs is about 0.122 mili-Sievert per year in Mexico’s urban zones.

Speaker: Prof. Alejandro Ramírez (National University of Mexico)

Paper ID_79_MARTÍNEZ_T.doc ID_79_MARTÍNEZ_T.pdf

Poster Cartel-potasioSicilia.pdf

49 Precipitation and purification of uranium from rock phosphate

This study was carried-out to leach uranium from rock phosphate using sulfuric acid in the presence of potassium chlorate as an oxidant and to investigate the relative purity of different forms of yellow cakes produced with ammonia {(NH4)2U2O7 }, magnesia (UO3.xH2O ) and sodium hydroxide (Na2U2O7) as precipitants, as well as purification of the products with TBP extraction and matching its impurity levels with specifications of the commercial products. Alpha-particle spectrometry was used for determination of activity concentration of uranium isotopes (234U and 238U) in rock phosphate, resulting green phosphoric acid solution, and in different forms of the yellow cake from which the equivalent mass concentration of uranium was deduced. Likewise, atomic absorption spectroscopy (AAS) was used for determination of impurities (Pb, Ni, Cd, Fe, Zn, Mn, and Cu). On the average, the equivalent mass concentration of uranium was 119.38±79.66 ppm (rock phosphate) and 57.85±20.46 ppm (green solution) with corresponding low percent of dissolution (48%) which is considered low. The isotopic ratio (234U: 238U) in all stages of hydrometallurgical process was not much differ from unity indicating lack of fractionation. Upon comparing the levels of impurities in different form of crude yellow cakes, it was found that the lowest levels were measured in UO3.xH2O. This implies that saturated magnesia is least aggressive relative to other precipitants and gives relatively pure crude cake. Therefore, it was used as an index to judge the relative purity of other forms of yellow cakes by taking the respective elemental ratios. The levels of impurities (Fe, Zn, Mn, Cu, Ni, Cd and Pb) in the purified yellow cake were found comparable with those specified for commercial products.

Speaker: Mr ELSHAFEEA ABOWSLAMA (Sudan Atomic Energy Commission)

Paper ID_189_Elshafeea_publication.doc ID_189_Elshafeea_publication.pdf

Poster Precipitation_and_purification_of_uranium_from_rock_phosphate.pdf

50 Recent sedimentation rates and trace elements determined in cores from Pantanal, Mato Grosso do Sul, Brasil

The Pantanal, in the southwest part of Brazil, is one of the world’s largest freshwater wetland. This natural ecosystem has been affected due to urban contamination, irregular use of the land, tourism without control and excessive agricultural defensive utilization. In order to verify possible changes in this environment, a study was established in Pantanal da Nhecolândia, Mato Grosso do Sul, Brazil in 2006. Two sediment cores were collected in two small ponds in Nhumirim farm, Salina do Meio and Salina da Ponta and one core was collected in a pond in Firme farm, Salina Pedra do Sol. The sedimentation rate was determined using the 210Pb dating method. The sedimentation rates obtained for the three pounds are in agreement with other lacustrine system of the literature. The elements As, Ba, Br, Ce, Co, Cr, Cs, Eu, Fe, Hf, La, Lu, Na, Nd, Rb, Sb, Sc, Sm, Ta, Tb, Th, U, Yb, Zn and Zr were determined by instrumental neutron activation analysis technique – NAA. Their concentrations ranged from mg kg-1 to %. For validation methodology the reference materials Buffalo River Sediment (NIST SRM 2704) and Soil-7 (IAEA) were analyzed. The majority of the elements and rare earths analyzed showed concentrations lower when compared with shale and earth crust values. Factorial analysis, mode R, Cluster analysis and principal component analysis were applied for the data interpretation.

Speaker: Dr Sandra Damatto (IPEN - CNEN/SP)

Paper ID_90_Damatto_Palermo_2011_final.doc ID_90_Damatto_Palermo_2011_final.pdf

Poster Damatto_Poster_Palermo_2011.pdf

51 Removal of volatile, organic iodines from vented containment gas streams by wet-scrubbing during severe nuclear accidents

During severe nuclear accidents several hazardous and radiotoxic gaseous fission products can be released and constitute a threat to the environment. Significant amounts of the radiotoxic fission product iodine, mainly as particular caesium iodide and gaseous elemental iodine, are released into the containment and coolant system assuming a core melt down accident. The distribution of iodine species in the containment follows a series of complex processes. Considerable amounts of gaseous iodine will dissolve in the water pools, condensing steam or water sprays and be converted into non-volatile species such as iodide and iodate ions. Remaining gaseous elemental iodine can react in numerous complex reactions with volatile organic substances like hydrocarbons released from organic materials such as cable isolations to form iodo-organics. Thus highly volatile airborne organic iodine species like methyl iodide and ethyl iodide can be formed from e.g. the reaction of methane with iodine. In e.g. Swedish light water reactors gaseous iodine species in excess gas streams being vented from the containment in case of a pressure increase are scrubbed off with an alkaline sodium thiosulfate solution. The removal efficiency for volatile iodo-organics is about 20 times lower than for elemental iodine. Those species of the isotope I-131 have a high potential to cause biological harm to humans by bioaccumulation when getting released to the environment due to their long enough half-life of app. 8 days. In response to improve the removal efficiency a modified scrubber solution has been developed containing nucleophilic organic compounds to achieve a rapid break of the organic iodines into non-volatile inorganic iodides maintaining in the scrubbing solution.

Speaker: Mrs Sabrina Tietze (Chalmers University of Technology)

52 Secure and certify studies to work on production of "spiked" plutonium

-In the nuclear weapons sites , work on materials include non nuclear testing of components of weapons that are sitting in the sites that include fundamental physics and engineering experiments on plutonium and investigating technologies for remanufacture of plutonium parts innuclear weapons and work on prodution of spiked plutonium which incorporates more of the isotope plutonium 238 than would normally be found in weapons -grade plutonium, 7.5 % rather than the typical 0.036 % . As plutonium 238 is more radioactive ,the spiking process accelerates the formation of defects that occur within the metal during alpha decay of plutonium ,the new alloy ages more quickly , on the equivalent of 16 years for every year of actual aging, which makes it perfect for experiments on plutonium decay, If typical weapons-grade plutonium , plutonium 239 is spiked with some plutonium 238 , which decay more quickly , the self-irradiation process dramatically picks up speed . If 5% of plutonium 239 is replaced with plutonium 238 , the sample will age 11 times faster than normal plutonium 239 .Aging can be accelerated by a faster of 16 over normal aging processes if 7.5% of the sample is plutonium 238. A useful measure of acceleration aging is defined as the number of years required to reach a radiation dose that results in 10 displacements per atom. Weapons-grade plutonium normally takes 100 years to reach this dose but will need just 6.25 years if it is spiked with 5% plutonium 238. In this paper(oral only), I discuss and present the advanced studies to certify a weapons test that shake , drop, heat and cool sample of fissile materials take place inside the test building.

Speaker: Prof. Prof.Dr.Mr.Ashraf Elsayed Mohamed Mohamed (Institute for Nuclear Materials)

53 Study of lactose uptake rate by immobilized kefir cells during whey fermentation, using C-14 labelled lactose

Whey or milk plasma is the liquid by-product of cheese processing units. Due to its high organic load of 40-70 g/L BOD5 and 60-80 g/L COD, whey represents an important environmental problem, especially in Greece, where about 700.000 tones whey are produced annually. Additionally, whey contains significant amounts of lactose and therefore it is suitable for further treatment, in order to produce useful fermented products like alcohol. Kefir is a natural mixed culture consisting of various yeasts (Kluyeveromyces, Candida, Saccharomyces, Pichia) and lactic acid bacteria of the genus Lactobacillus. It has been found that yeasts and lactic acid bacteria co-exist in a symbiotic association in kefir and are responsible for lactose fermentation of milk and whey. Also, the positive effect of kefir cell immobilization on organic or natural supports in whey fermentation rate has been confirmed and the most acceptable explanation for this was the enhancement of catalytic action of some enzymes involved in the process. However, due to the fact that fermentation rate depends on lactose uptake rate by microorganisms, research efforts have been undertaken in order to study kefir fermentation ability. So, tracers have been used to record lactose uptake rate by kefir as labelled and unlabelled molecules of the same compounds species follow the same metabolic pathways. In the present work 14C-labelled lactose was used to study lactose uptake rate by kefir cells immobilized on delignified cellulosic (DC) materials, gluten pellets and brewery spent grains (BSG), during whey fermentation, in order to reveal the role of uptake rate in the promotional activity of these supports. Results illustrated that whey fermentation by immobilized kefir cells was faster compared to free cells and in case of DC materials, fermentation time was found only 7.2 h. Also, the lactose uptake rate by kefir immobilized on DC materials was higher compared to other supports.

Speaker: Aristidis golfinopoulos (university of patras)

54 Study of states of uranylphosphates and uranylarsenates of monoacid, divalent and trivalent elements in water-salt heterogeneous systems

The state of compounds of general formula Ak(BvUO6)k•nH2O (Ak - alkaline, alkaline earth, 3d-transition and rare earth elements; Bv - P, As) in aqueous solutions in the wide range of pH 0-14 was investigated. The acid-base range of existence of uranylphosphates and uranylarsenates was established, products of conversion were identified and the solubilities of these compounds were determined. Using of the obtained data and the instrument of equilibrium thermodynamics, the solubilities of products, Gibbs’s functions of formation of the compounds Ak(BvUO6)k•nH2O and solubility curves were calculated, diagrams of the state of uranium (VI) and arsenic (V) in solution and equilibrium solid phases were constructed. It was established that the behavior of all compounds Ak(BvUO6)k•nH2O in aqueous solutions obeys to common foundations due to their structure and chemical properties similarity of phosphorus and arsenic. Acidity has the most significant influence on the state of studied compounds in the water-salt heterogeneous systems. Generally uranylphosphates are chemically more stable than uranylarsenates. That conclusion one can prove by wider acid-base ranges of their existence and the lower solubility. Derivatives of alkaline and alkaline earth elements in both families of compounds hold their composition and structure interacting with aqueous solutions in wide range pH 2-11, whereas uranylphosphates and uranylarsenates of lead, 3d-transition and rare earth elements save their individualities in more narrow range of pH 2-8. It was shown that the solubilities of all uranylphosphates and uranylarsenates are minimal in the neutral solutions and increases after transition into acid and base media. In the general case solubilities of uranylphosphates and uranylarsenates at the same pH decreases with increasing of the interlayer atom radius.

Speaker: Dr Oxana Nipruk (Nizhni Novgorod state University)

55 Study of the firing temperature of Marajoara Archaeological ceramics by electron paramagnetic resonance associated to INAA data

The Marajo Island is the largest island of the Marajo archipelago, located in the North of Brazil. With an area of approximately 50,000 km2, it is located in the Para State and east part of the Amazon. In this region, at the end of 19th century, it was identified an archaeological society named Marajora, which occupied the island from 400 to 1400 AD. It was characterized by the development of an intensive subsistence system based on fish farming and by a ceramic style recognized by its beauty and exuberance. Until this moment, the physical and chemical analysis studies in this ceramics are scarce and this kind of studies may help to archaeological studies made in the island. With this purpose, this work presents a preliminary study of the firing temperature in the ceramics. For that, the elementary concentrations of 100 samples from Museu de Arqueologia e Etnologia of São Paulo University and samples collected in the Marajo Island were studied. The samples were analyzed using instrumental neutron activation analysis in which the elemental concentration of Ce, Co, Cr, Cs, Eu, Fe, Hf, K, La, Lu, Na, Nd, Rb, Sc, Sm, Ta, Tb, Th, U, Yb and Zn were determined. The interpretation of the results was made using principal components analysis and showed the existence of three chemical groups. Some samples of each cluster were chosen for the determination of their firing temperatures by electron paramagnetic resonance, in order to verify if different firing temperatures was associated with different elemental groups of ceramic samples. The results showed no statistical differences in the firing temperature between the samples from Museu de Arqueologia e Etnologia and the samples collected in the Marajo Island.

Speaker: Ms Kelly Nunes (Instituto de Pesquisas Energéticas e Nucleares)

Paper ID_88_Paper.doc ID_88_Paper.pdf

Poster ID_88_Poster.pdf

56 Synthesis and study of uranyl orthovanadate (UO2)3(VO4)2*4H2O

Uranyl orthovanadate (UO2)3(VO4)2•4H2O was synthesized by heating of uranyl divanadate, (UO2)2V2O7. Structure of this compound was studied with X-ray fluorescence analysis, high temperature X-ray diffraction, scanning calorimetry, IR-spectroscopy. X-ray and IR characteristics of products of its dehydration were determined. Synthesis has consisted of uranyl divanadate (UO2)2V2O7 heating in aqueous solution at pH 7 for 48 hours in hydrothermal conditions at 200oC. 200oC 3(UO2)2V2O7+8H2O→2(UO2)3(VO4)2•4H2O+V2O5 Admixture of free V2O5 has been deleted by washing of precipitate with ammonium aqueous solution at 50oC. The results of chemical analysis showed that obtained compound is tetrahydrate 3UO3•V2O5•4H2O. X-ray data for the compound indicates that it is crystallographic analogue of the known uranyl orthovanadate (UO2)3(VO4)2•5H2O. Part of molecular H2O is weakly associated and water molecules do not fill crystallographic positions by themselves and conversion (UO2)3(VO4)25H2O → (UO2)3(VO4)24H2O does not lead to any significant changes of crystal lattice. Dehydration of tetrahydrate in wide temperature range (70-325oC) includes some stages. The crystal lattice of anhydrous composition (UO2)3(VO4)2 holds its layered structure with special set of crystallographic characteristics. However, dehydration is reversible. Compound is hydroscopic and its cooling leads to absorbing of three molecules H2O from air with subsequent returning into the original crystalline state. Addition of the fourth water molecule takes place after direct contact with aqueous phase at temperature that is not more than 20oC. IR-spectrum of (UO2)3(VO4)24H2O is very characteristic and informative. There are well expressed three groups of vibrations. We have found vibrations of water molecules, uranyl group UO22+ and vanadate tetrahedra. Form of water vibrations one could conclude that all water molecules hold their vibration individuality. From the results obtained it was concluded that compound (UO2)3(VO4)2*4H2O belongs to the family of uranium derivatives with the layered type of crystal lattice.

Speaker: Ms Anna Eremina (Nizhni Novgorod state University)

57 Test of isotopic exchanges between O-18 and O-16 when oxygen-18 enriched water contacts with air oxygen

Nowadays, 2-deoxy-2-D-glucose radiolabeled with Fluorine-18 (18FDG) is widely used in cancer imaging studies as a popular PET radiopharmaceutical. For synthesis of 18FDG, 18F radionuclide is first produced by 18O (p, n) 18F nuclear reaction in a Medical Cyclotron. For this nuclear reaction, 18O enriched water (H218O) with about 97 % enrichment level is used as a target material in the Medical Cyclotrons. The main purpose of this study was to investigate the probable exchanges between 18O and 16O isotopes when H218O contacts considerably long time with air Oxygen. Thus, it would be determined that H218O should be avoided to contact with air Oxygen and to keep in an inert gas for long time storages or not. For this experiment, natural Oxygen and Argon gases were separately passed through H218O with 1 % 18O enrichment during long times up to about 8 days. Samples of about 1.5 mL taken from H218O with 1 % 18O enrichment have been analyzed by Isotopic Ratio Mass Spectrometry (IR-MS) technique in England. 18O analyses have showed that air Oxygen contact causes the decrease of 18O / 16O ratio and contrarily, Argon contact causes the increase of 18O / 16O ration. This means that H218O should be avoided to contact air Oxygen and during long time storages H218O is recommended to keep under an inert atmosphere like Argon. Otherwise, the enrichment level of H218O may considerably be decreased.

Speaker: Mrs Selen Ekim (Ege University, Faculty of Science, Department of Chemistry, Division of Nuclear Chemistry, Bornova, Izmir 35100, Turkey)

Paper ID_163_2_Selen_O-18_(Full_paper).doc ID_163_2_Selen_O-18__Full_paper_.pdf

58 The distribution of I-131 in the fractionated dust in the ground layer of air in central Poland

March 11, 2011 as a result of earthquakes and tsunamis the reactor No. 1 in Fukushima Dai-ichi in Japan has been breakdown. As a consequence of failure the release of significant amounts of radionuclides such as I-131, Cs-137, Cs-134, Te-131 and the other to the atmosphere was observed. Emitted isotopes were transported with air masses even at considerable distances. The concentrations of some these radionuclides were also observed over the Polish territory. The highest concentrations of I-131 (about 8 mBq/m3) was observed in the central part of the Polish, the third week after the accident. The maximum observed concentrations of Cs-137 and Cs-134 was 0,75 and 0,61 mBq/m3, respectively. In order to verify the exact radiological consequences of I-131 inhalation it is important to know their distribution in air particulate matter. The highest concentration of I-131 [μBq/m3] is observed for the smallest aerosols, with diameter lower than 1 μm (filter number 9-this value is twice higher of that for bigger fractions in range from >2 μm). As we expect I-131 is predominantly linked to small and mobile fraction of aerosols. Information about the distribution of concentrations in different fractions of aerosols can be used to estimate the rate of spread of the radionuclides. In addition, it is possible to estimate the delivered dose for the occupants of the various regions. Monitoring the transport of radionuclides in the atmosphere is an important element of radiological exposure assessment. It should be emphasized that the observed isotope concentrations in the air in the central part of the Polish were not dangerous for the residents, but their observation is an excellent test of the efficiency of use monitoring systems.

Speaker: Mr Paweł Grabowski (Technical University of Lodz)

59 The effect of aging and natural organic matter on the Th(OH)4 solubility

The formation and solubility of the Th(OH)4 solid phase has been investigated as a function of the aging time and the presence of natural organic matter (e.g. humic acid) in 0.1 M NaClO4, in the pH range between 2 and 5, and under normal atmospheric conditions. Th(OH)4 has been prepared by alkaline precipitation and characterized by TGA, ATR-FTIR, XRD, and solubility measurements. According to the experimental data Th(OH)4 is stable and remains the solubility limiting solid phase even in the presence of increased humic acid concentration in solution. Increasing humic acid concentration doesn’t affect the crystallite size and the solubility product of Th(OH)4 and its solubility is basically pH depended and governed by the presence of colloidal species. However, solid phase aging, which in absence of humic acid favors crystallinity, affects significantly the Th(OH)4 solubility. Keywords: Th(IV); solubility; humic acid; aging; particle size

Speaker: Ms Melpomeni Prodromou (University of Cyprus)

Paper ID_101_The_Effect_of_Aging_and_Natural_Organic_Matter_on_the_Th(OH)4_Solubility.doc ID_101_The_Effect_of_Aging_and_Natural_Organic_Matter_on_the_Th_OH_4_Solubility.pdf

Poster MELPO_POSTER_SICILY_2011.pdf

60 The effect of humic acid on the formation and solubility of secondary solid phases of polyvalent metal ions

The paper presents and discusses data obtained from investigations regarding the effect of natural organic matter (e.g. humic acid) on the formation and solubility of secondary solid phases of polyvalent metal ions (e.g. M(VI), M(IV), M(III)) in aqueous solutions of 0.1 M NaClO4 and under normal atmospheric conditions. The investigations were performed using hexavalent uranium as analogue for M(VI), tetravalent thorium, cerium and zirconium as analogues for M(IV) and trivalent samarium and neodymium as analogues for M(III). The solid phases under investigation have been prepared by alkaline precipitation in the presence and absence of humic acid and characterized by TGA, ATR-FTIR, XRD and solubility measurements. The experimental data obtained indicate generally that the solids phases, which are formed in the absence of humic acid, are stable and remain the solubility limiting solid phases even in the presence of increased humic acid concentration (up to 0.5 g/l) in solution. Although polyvalent metal ions form very stable complex with humic acid, upon base addition in the M(z)-humic acid system decomplexation of the previously formed M(z)-humate complexes and precipitation of two distinct phases occurs, namely, the inorganic and the organic phase. The latter is adsorbed on the particle surface of the former. However, natural organic matter (humic acid) affects the particle size of the solid phases and may lead to reduction of redox-sensitive species. Generally, increasing humic acid concentration results in decreasing crystallite size of the inorganic solid phase. The extent of the effect depends inversely on the solid phase stability. The impact on the solid phase properties even for the less stable solid phases is expected to be of minor relevance regarding the chemical behavior and migration of polyvalent metal ions in the geosphere. Keywords: polyvalent metal ions, humic acid, solid phase formation, solubility

Speaker: Dr Stella Antoniou (University of Cyprus)

Paper ID_102_AntoniouS._full_paper_doc.doc ID_102_AntoniouS._full_paper_doc.pdf

Poster POSTER_STELLA_SICILY_new.pdf

61 The granular sorbents for passive environment protection system during severe accidents with total loss of power supply at NPPs

The problem of reliable environmental protection measures in the event of severe nuclear power plant accidents appears to be an important factor restraining the development of nuclear energy. It is known that a hypothetic severe accident accompanied by a partial or complete destruction of the reactor’s active zone, bring about the formation of large quantities of gaseous products. This leads to an abrupt increase in pressure inside the containment and there is a risk of its destroying. For decreasing of the pressure inside the containment, the some nuclear power plants are equipped with pressure release system. The modern designs of new-generation nuclear power plants with two protective shells do not provide for pressure release systems [1 - 3]. It is planed that during hypothetical severe accidents all radioactivity will be localized inside containment. To prevent radioactive contamination of the environment, modern designs are equipped with active venting filtering systems, which require regular electric power supply. However, in accordance with the general requirements for safety systems, alongside active ventilation systems for intercontainment space, nuclear power plants should include a passive ventilation system, which can be used during hypothetical severe accident with a complete loss of power supply. Based on the fundamental studies on localization of volatile fission products the new passive environment protection system during severe accidents at new generation NPPs is suggested. The basic purpose of developed passive filtration system is creation of a rarefaction in an intercontainment space due to the organized removal of the radioactive steam-air mixture from an intercontainment space at full loss of all power sources. Steam-air mixture containing radioactive aerosols and flying fission products removal from an intercontainment space is passed through the special filtering module. Efficiency of cleaning of a radioactive steam-air mixture is determined by filtration and sorption properties of used filtering elements. On the basis of fundamental researches on localization of molecular and organic forms of radioactive iodine from a steam-air flow in operating conditions of passive filtering system during severe accidents the granulated sorbents "Fizkhimin"TM, containing particles of Ag or Ag-Ni compounds with nanometric sizes, were selected for given filtering module. The granulated sorbent "Fizkhimin"TM represents silica impregnated by Ag or Ag-Ni and modified on technique of IPCE RAS. The sorbent is issued as several types and represents granules of dark color with the sizes of particles 0.5-6.0 mm. The studies of sorbent properties have shown, that it radiationally stable at a doze 500 MRad and does not initiate ignition of hydrogen. The given sorbents have high sorptive efficiency in relation to molecular iodine and iodide methyl. At that it is necessary to note, that they do not lose the sorptive efficiency up to temperature 300oC and up to temperature 600oC from them does not occur the desorption of radioactive iodine in a gas phase. Taking into account novelty of development and an opportunity of the international application of passive filtering system (the Russian project of the NPP WWER-1000 in India), expert international tests of efficiency of sorbents "Fizkhimin"TM based on Ag nanometric compounds on absorption of volatile radioactive iodine compounds at the stand of "ТUV Energie und System Technic" (TUV ET) (Karlsruhe, Germany) have been carried out. Testing passed on localization most difficult sorptive form of the radioactive iodine - methyl iodide. Results of tests have shown that sorbents have very high sorptive efficiency relative to most difficult localize form - to methyl iodide, at various experimental parameters. In conclusion, it is necessary to note, that the granulated sorbents "Fizkhmin"TM have very high sorptive efficiency in a wide range of experimental parameters and consequently they can be used for localization of volatile radioactive iodine compounds not only in passive filtering system, but also in other filtering devices, for example in the filters of emergency pressure release from containment operational NPPs during severe accidents. Work is supported by Council about grants of the President of the Russian Federation for the state support of leading scientific schools of the Russian Federation (grant SS-6692.2010.3). References 1. "Reactor Design" // Nucl. Engin., 2002, Advert. Supplement. 2. Krebs, W.-D. "The New Generation" // Siemens Power J., 1999, no. 4, p. 10 - 13. 3. "Tomorrow's reactors" // Alternatives, 2003, no. 2, p. 4-5.

Speaker: Prof. Sergey Kulyukhin (Institute of Physical Chemistry and Electrochemistry RAS)

Paper

• ID_2_Kulyukhin.doc
• ID_2-Kulyukhin.pdf
• ID_2_Kulyukhin.pdf

Poster Poster_ID_2-Kulyukhin.pdf Poster_ID_2-Kulyukhin.ppt

62 The thermal decomposition of CH3131I in a gas flow

The localization of volatile radioactive iodine compounds by various sorbents from vapor-gas media is a vital issue for environmental protection during both irradiated nuclear fuel reprocessing and accidents at nuclear power enterprises, including nuclear power plants (NPPs). The work studies the thermal decomposition of methyl iodide CH3131I, a volatile radioactive iodine organic compound, in a gas flow in the presence of various modifications of "Fizkhmin"TM granulated materials based on silica gel impregnated with d-elements. Test facility concluded the following basic parts: rotameters (1); a CH3131I generator (2); scrubber with water (3); the heating furnace of mine type (4); composite materials under study (5); the thermocouple (6); a column with SiO2-Cuo (7); scrubber with 0.05 M Na2SO3 solution (8); the heating furnace of tubular type (9); columns with SiO2-AgNO3 (10). The study found that in the absence of "Fizkhmin"TM material, the degree of the decomposition of CH3131I (10 mg) in air (flow rate 4.5–5.5 cm/s and time of the air flow presence in the heating zone 1.0 – 1.5 s) was equal to (7-10)% at (540  10)оС, ~(70-75)% at (640  10)оС, and ~(97-99)% at (770  15)оС. In the presence of silica gel granules measuring 1.0-3.0 mm, the degree of the decomposition of CH3131I (10 mg) in air (linear flow rate 4.8–5.2 cm/s and time of the air flow presence in the heating zone 1.0–1.1 s) was equal to (2-3)% at (240  10)оС, ~(10-15)% at (340  10)оС, ~(75-80)% at (440  10)оС, and ~(97-99)% at ~(540  10)оС. Silica gel granules allow decreasing the CH3131I thermal decomposition temperature in an air flow by ~200оС. In the presence of "Fizkhmin"TM granulated materials impregnated with Ni compounds or Ni-Cu mixture (8-10 wt.% and granule size 1.0–3.0 mm), the degree of the decomposition of CH3131I (10 mg) in air (linear flow rate 4.8–5.2 cm/s and time of the air flow presence in the heating zone 0.8–1.1 s) was equal to <0.2% at (20  3)оС, ~(0.3-1.0)% at (150  20)оС, (15-30)% at (250  10)оС, ~(85-92)% at (340  15)оС, and ~(95-99)% at (465  20)оС. "Fizkhmin"TM granules containing 8-10 wt.% Ni or its mixture with Cu, allow decreasing the CH3131I thermal decomposition temperature in an air flow by more than ~300оС. The work studies the dependence of the CH3131I thermal decomposition degree on the concentration of a d-element in the "Fizkhmin"TM material and its storage time, as well as on the amount of CH3131I in an air flow. Work is supported by Council about grants of the President of the Russian Federation for the state support of leading scientific schools of the Russian Federation (grant SS-6692.2010.3).

Speaker: Prof. Sergey Kulyukhin (Institute of Physical Chemistry and Electrochemistry RAS)

Paper

• ID_3_Kulyukhin.doc
• ID_3-Kulyukhin.pdf
• ID_3_Kulyukhin.pdf

Poster Poster_ID_3-Kulyukhin.pdf Poster_ID_3-Kulyukhin.ppt

63 Unconventional component of parent materials of moldavites

Formation of the Central European tektites - moldavites - has unequivocally been associated with a large meteorite impact to Ries region in western Bavaria in Germany 14.5 million years ago. However, after several decades of investigation, unambiguous assigning all source materials of moldavites and processes of their chemical differentiation still remains open. Despite some similarity of chemical composition between moldavites and isochronous sediments from vicinity of the Ries crater, there are some significant differences in both major and trace element contents, which cannot be attributed solely to the variability of sediments or later weathering processes. Geochemical characterization of a large collection of moldavites using various modes of instrumental neutron and photon activation analyses supported a novel hypothesis, according to which ash from biomass burned at the early stage of the meteorite impact contributed to the source materials. As shown by the geochemical data acquired in the study, this unconventional “biogenic component” could be indicated by enrichment in elements essential for plants (e.g., K, Ca, Mg) and depletion of nonessential elements (e.g., Na, Rb, Sr, Ba), similarly to redistribution of these elements during their transfer from soil to plants. Differentiation similar to that occuring during the soil/plant interaction has been observed also for other, nonessential elements, e.g., U and Th. Correlations between the K/Na ratio and Ca/Sr, Ca/Ba, K/Rb, U/Th ratios, as well as some other indicators of the “biogenic component” observed in moldavites from various parts of the Central European tektite strewn field are presented and discussed. This study has been supported by the Czech Science Foundation grant 205/09/0991.

Speaker: Dr Jiří Mizera (Nuclear Physics Institute ASCR)

Poster 158_Mizera-poster.ppt

64 Uranium in dog foods commercialized in Brazil

Commercial dog food is supposed to be a complete and balanced diet, formulated by mixing several ingredients, aiming at being the exclusive source of all nutrients for a healthy life of dogs. However, for reducing costs, low quality ingredients are often used in the composition of dog food, including byproducts from meat and grain processing and byproducts from other food industries, as well as mineral substances. Low quality ingredients can introduce residues of pesticides, mycotoxins and other toxic substances, like uranium, causing health problems to the animals. The overexposure to uranium may cause pathological alterations in the kidneys. In this context, the objective of this work was to further investigate the presence of uranium in dry dog foods of various brands commercialized in Brazil. Thirty-four samples, including food for puppies and adults, were acquired in the local market of Piracicaba. The dog food samples were ground in titanium knife mill, homogenized and evaluated by instrumental neutron activation analysis (INAA). The results were expressed in dry mass basis. The U concentration ranged from <0.46 to 3.99 mg/kg, with the three highest values for the same brand (2.07 mg/kg, 3.15 mg/kg and 3.99 mg/kg). Furthermore, there were correlation between U and Sc (R=0.968) and U and La (R=0.617). Such correlations indicated that the high values of uranium originate from mineral ingredients or from contamination with geological material, since Sc and La are rare earth elements used as tracers of geological material. Uranium is naturally present at high levels in some phosphate rocks, which are the main economically viable source of phosphorus, widely used for the production of fertilizers, and for animal nutrition.

Speaker: Ms Camila Elias (University of São Paulo / Center of Nuclear Energy in Agriculture / Radioisotopes Laboratory)

65 Uranium in ground water samples of Northern Greece

The activity concentrations of 238U and 234U have been determined in groundwater samples of hot springs and deep wells in Northern Greece. The analysis was performed by alpha spectroscopy after pre-concentration and separation of uranium by cation exchange (Chelex 100 resin) and finally its electro-deposition on stainless steel discs. The uranium concentration in deep wells and springs varies strongly between 0.15 and 7.66 μg l-1 and the corresponding 238U and 234U activity concentrations between 1.82-95.3 mBq l-1 and 1.70-160.1 mBq l-1 respectively. The obtained isotopic ratio 234U/238U varies between 0.95 and 1.74 indicating a disturbed radioactive equilibrium between the two uranium isotopes. In the studied waters uranium concentrations in solution decrease with increasing pH in the pH range between 7 and 9. This is attributed to the fact that at lower pH dissolution of soil minerals occurs and uranium which is adsorbed or forms solid solution with the geological matrix enters the aqueous phase. The strong dependence of the uranium concentration in the studied waters from the dissolution of the geological matrix is corroborated by the strong correlation of the uranium concentration with the electrical conductivity measured in the ground waters under investigation.

Speaker: Prof. ALEXANDRA IOANNIDOU (ARISTOTLE UNIVERSITY OF THESSALONIKI, Physics Department, Nuclear Phys. & Elementary Particle Phys. Division)

Dinner - not included

Tuesday 20 September

Session 5: Radioecology and Geochemistry

66 Half-lives of Pu isotopes

Speaker: Prof. Suresh Aggarwal (Homi Bhabha National Institute (HBNI))

67 Half-lives of nuclides for geological use: 2011 evaluations for U-235 and U-234

The IUPAC-IUGS joint Task Group “Isotopes in Gesciences”, TGIG, has evaluated the published measurement results for decay constants (i.e. half-lives) of U-235 and U-234 relative to that of U-238. A measurement result is generally expressed (VIM, 2008, entry 2.9) as a single measured quantity value and a measurement uncertainty. A significant part of the present evaluation was the assessment of the measurement uncertainties following strict metrological criteria (GUM, 2008). Following the counting experiments by Jaffey et al. (1971), which yielded the U-238 half-life still deemed reliable, albeit with a higher uncertainty, the endeavor in the geochronological community (Schoene et al., 2006; Mattinson, 2010) moved to determining the U-235 half-life indirectly, based on U-Pb dating of single crystals of zircon (natural ZrSiO4). The approach is based on the assumption that certain natural samples behave “ideally”, i.e. their 238U-206Pb and 235U-207Pb ages (hereafter t-206 and t-207, respectively) are expected a priori to be equal. However, in current practice only the concentration N(U-238) is measured at present, and the concentration N(U-235) is calculated assuming a constant number ratio eta = N(238U)/N(235U) = 137.88. Recent reports on etameasurements in magmatic rocks (Weyer et al., 2008) indicate that granites and basalts, typical magmatic rocks used for geochronology, have an eta lower by (0.031 ± 0.011)% relative to the NIST standard reference material SRM 950a. In turn, the latter was measured by Condon et al. (2010), who report eta = 137.847 ± 0.012. Combining these two recent re-determinations, the typical granitic zircon grains used for geological sample intercomparisons are predicted to have eta = 137.804 ± 0.021. From these, we calculate a provisional value for the 235U half-life of (703.44 ± 0.23) Ma (1s uncertainty), corresponding to lambda-235 = (0.98537 ± 0.00032) Ga-1. The 234U half-life (Cheng et al., 2000) was obtained following strict material traceability protocols, and had the explicit goal of ensuring the radioactive equilibrium of natural samples. The etanumber-ratios of the NBL CRM 112a and U-500 reference materials that they used as spike and dectector calibrators were subsequently revised (Condon et al., 2010). In particular, recalculating etain Cheng et al.’s (2000) spike using Condon et al.’s (2010) revised etafor U-500 also accounts for a shift in the eta for NBL CRM 112a. As a consequence, the half-life is modified by + 0.07 % to (245.44 ± 0.16) ka (1s uncertainty), corresponding to lambda-234 = (2.8241 ± 0.0018) Ma-1. Cheng H., Edwards R.L., Hoff J., Gallup C.D., Richards D.A., Asmerom Y. (2000) The half-lives of uranium-234 and thorium-230. Chem. Geol. 169, 17-33. Condon D., McLean N., Noble S.R., Bowring S.A. (2000) Isotopic composition (U-238/U-235) of some commonly used uranium reference materials. Geochimica et Cosmochimica Acta 74, 7127-7143. GUM (2008) Guide to the expression of uncertainty in measurement. www.bipm.org/en/publications/guides/gum.html Jaffey A.H., Flynn K.F., Glendenin L.E., Bentley W.C., Essling A.M. (1971) Precision measurement of half-lives and specific activities of 235U and 238U. Phys. Rev. C4, 1889-1906. Mattinson J. (2010) Analysis of the Relative Decay Constants of 235U and 238U by Multi-step CA-TIMS Measurements of Closed-System Natural Zircon Samples. Chem. Geol. 275, 186-198. Richter S., Alonzo-Muñoz A., Eykens R., Jacobssen U., Kuehn H., Verbruggen A., Aregbe Y., Wellum R., Keegan E. (2008) The isotopic composition of natural uranium samples—measurements using the new N(233U)/N(236U) doublespike IRMM-3636. Internat. J. Mass Spectrometry 269, 145-148. Schoene B., Crowley J. L., Condon D. J., Schmitz M. D., Bowring S. A. (2006) Reassessing the uranium decay constants for geochronology using ID-TIMS U-Pb data. Geochimica et Cosmochimica Acta 70, 426-445. VIM (2008) The International Vocabulary of metrology – Basic and general concepts and associated terms, 3rd edition, JCGM 200:2008, http://www.bipm.org/en/publications/guides/vim.html Weyer S., Anbar A.D., Gerdes A., Gordon G.W., Algeo T.J., Boyle E.A. (2008) Natural fractionation of 238U/235U. Geochim. Cosmochim. Acta, 72, 345-359.

Speaker: Prof. Igor Villa (Institut für Geologie, Universität Bern, CH-3012 Bern, Switzerland; Dipartimento di Scienze Geologiche e Geotecnologie, Università di Milano Bicocca, I-20126 Milano, Italy)

68 Radioecology around a closed uranium mine

Uranium mine at Žirovski vrh, Slovenia, operated from 1985 to 1990 and processed about 600,000 tons of uranium ore. The uranium mill tailings (UMT) were deposited onto the Boršt waste pile lying close to the mine, in the subalpine region with relatively high rainfall and within a relatively densely populated area. The mining influential area has been under continuous radiological monitoring since starting industrial excavations in 1982. However, more detailed radioecology studies were initiated some six years ago. They are focused on assessing mobility and bioavailability of radionuclides present in the tailings pile. The mobility of 238U, 234U, 230Th and 226Ra was studied by the Shultz modified Tessier sequential extraction procedure. The uranium isotopes were found to be the most mobile from the UMT, whilst the mobility of 226Ra and 230Th appeared to be suppressed by high sulphate concentrations. When comparing the revised BCR and the modified Tessier sequential extraction protocols it was found that the protocols are not comparable as the data obtained are protocol- and element- dependent. Uptake of particular radionuclides by the plants grown in the vicinity of the former mine were also investigated. In particular, a common reed grown in soils contaminated with the seepage waters from the tailings was studied. The plants contained elevated levels of 238U, 226Ra and 210Pb compared to the plants from control site. Activity concentrations of natural radionuclides in milk collected from the area of Žirovski vrh were comparable to the reference location, except of uranium where the content was higher. The combined annual effective dose for adults consuming milk from the Žirovski vrh area is 13.0 ± 1.7 μSv/year.

Speaker: Dr Borut Smodiš (Jožef Stefan Institute)

Paper ID_10_Smodis.doc ID_10_Smodis.pdf

69 Uranium isotopes as a tracer of groundwater transport studies

The uranium chain radionuclides are usually used for a wide range of application in the Earth Sciences. The 234U/238U activity ratio is used as a geochemical tool to investigate transport and flow relationships in major hydrological reservoirs, groundwater pattern and it is highly useful for interpreting timescales of weathering. In rocks older than a few million years, 234U/238U activity ratios should be in secular equilibrium. Nevertheless, the highly energetic alpha decay of 238U damages a mineral’s crystalline lattice and allows 234U to be more mobile during weathering of rock by atmospheric water [1]. In this work, the activity concentration and isotopic ratio of uranium isotopes (234U/238U) were determined in selected thermal groundwater, ground and surface water samples from central Poland. Additionally the radionuclides concentration in one sample of thermal groundwater from southwest Poland were determined. Uranium isotopes after co-precipitation with hydrated manganese dioxide were separated from other natural radionuclides by extraction chromatography resin (Dowex 1x8). The activity concentrations were determined by using α spectrometry with PIPS detector (Camberra). Concentration of 234U and 238U in the examined waters varied from 0.75 mBq/dm3 to 16.8 mBq/dm3 and from 0.64 mBq/dm3 to 45.5 mBq/dm3 respectively. The highest uranium concentrations were measured in the thermal groundwater from Mszczonow and Cieplice, while the lowest were observed in ground water from Plock which are got out from Cretaceous geological formation. The 234U/238U activity ratio varied from 0.370 (Cieplice) to 1.205 (Plock – Tertiary geological formation). It confirms that the uranium isotopic ratio can be useful indicator for determination of surface water infiltration input into the underground water reservoirs. [1] Camacho A., Devesa R., Valles I., Serrano I., Soler J., Blazquez S., Ortega X., Matia L.: J. Environ. Radioact. 101, 1048 (2010)

Speaker: Mr Paweł Grabowski (Technical University of Lodz, Department of Chemistry, Institute of Applied Radiation Chemistry)

70 U-238 in sediments of the Kastela Bay, Adriatic Sea (Croatia)

Distribution of U-238 in sediments of the Kastela Bay near the city of Split (Croatia) to a depth of 50 cm was studied due to an assumed discharge of the TENORM (Technologically Enhanced Naturally Occurring Radioactive Material) in the Bay. Sediment cores, comprising 604 samples, were taken on 95 stations and sliced into eight segments. U-238 massic activities were measured by gamma-spectrometry method using the Th-234 63.3 and 92.6 keV lines. Massic activities range was 6.7 – 603 Bq/kg, mean value 34 Bq/kg, median 28 Bq/kg and the standard deviation 46 Bq/kg in eight sediment layers of 0 – 50 cm depth. The maximum activity was determined in a layer 5 (20 – 25 cm depth) on the station next to a former chemical factory ”Adriavinil”. U-238 massic activities of the Kastela Bay sediments generally show values typical for marine sediments. However, some elevated U-238 activities were observed on five stations. Four stations are located around the Split peninsula and one next to the ”Adriavinil” factory. Moderately elevated massic activities (62 – 191 Bq/kg) were observed on stations around the Split peninsula and in the deepest layer (layer 7 at 30 – 40 cm depth) on the station next to the ”Adriavinil” factory. These activities were 3 – 10 times elevated compared to the activity of a typical Adriatic coast sediment (18.2 Bq/kg) and 1.5 – 5 times compared to the activity of an uncontaminated average Kastela Bay sediment (38.8 Bq/kg). Very elevated massic activities (392 – 603 Bq/kg) were registered only on the station next to the ”Adriavinil” factory in the layers 1 – 6 (0 – 30 cm depth). Compared to the activity of the typical Adriatic coast sediment, activities in six layers on this station are 22 – 33 times elevated and 10 – 16 times compared to the activity of the uncontaminated average Kastela Bay sediment.

Speaker: Dr Ivanka Lovrencic Mikelic (Rudjer Boskovic Institute)

Slides 3rd_INCC_-_Ivanka_Lovrencic_Mikelic.pdf

71 Plutonium speciation during sorption on natural clay

Plutonium will be a major contributor to the radiotoxicity of spent nuclear fuel after storage times of more than 1,000 years due to the long half-lives of Pu-239 and Pu-240. Several European countries are considering argillaceous rocks as potential host rock formation for high-level nuclear waste repositories. Plutonium has a very rich and complex chemistry in aqueous solution, where up to three Pu oxidation states can coexist. Therefore, detailed studies on the migration behavior of Pu are required for assessing the safety of deep geological disposal of nuclear waste in clay formations. We investigated the sorption of Pu in oxidation states III-VI on Opalinus clay (OPA, Mont Terri, Switzerland) using several synchrotron-based techniques: X-ray absorption fine structure spectroscopy (EXAFS, µXANES), X-ray fluorescence (µXRF), and X-ray diffraction (µXRD). Pu L3-edge EXAFS measurements on OPA suspensions showed that inner-sphere surface complexes of tetravalent Pu dominate its speciation in the clay, independent from the initial Pu oxidation state in the aqueous phase. Similar results have been observed previously for the sorption of Pu on kaolinite [1], which is with 22 ± 2% an important clay constituent of OPA. To determine which mineral phases of OPA are responsible for the uptake of Pu, thin sections of OPA bore cores were exposed to different Pu solutions and analyzed with high spatial resolution (≤ 1.5 µm) at the SLS MicroXAS Beamline. µXRF mapping revealed areas that were enriched in Pu. Pu-µXANES measurements showed that Pu(IV) is the major oxidation state in these areas. According to µXRD, clay minerals (kaolinite, illite), Fe(II) minerals (siderite, pyrite), calcite, and quartz dominate the mineralogy of the Pu-rich areas. [1] T. Reich et al., Application of XAFS to Actinide Environmental Science, AIP Conf. Proc. 882 (2007) 179.

Speaker: Prof. Tobias Reich (Johannes Gutenberg-Universität Mainz)

Slides Reich_3rdINCC.ppt.pdf

72 A system for radwaste storage real-time monitoring: lab and real tests

A prototype array of modular sensors for online monitoring of radioactive waste was developed at INFN-LNS. With the main purpose of counting gamma radiation, we implemented a new kind of mini-sensor, based on Silicon PhotoMultipliers and scintillating fibres, that behaves like a cheap scintillating Geiger-Muller counter. It can be replicated, for instance, in shape of a fine grid around each single waste drum in a repository. After simulating the counting response of thin scintillating fibers to gamma radiation, we verified our simulation results with precision measurements on the bench with laboratory sources. Front-end electronics and an FPGA-based counting system was developed, in order to handle the data flow coming from the field sensors. Such a system also deals with the redundant data transmission toward a console with a graphical user interface and a data storage system. The redundant transmission is done on differential cables and also foreseen wireless using low-power ZigBee units. The log data are foreseen to be stored onto a database system navigable by means of a web browser interface. A robotic arm demonstrator was developed and is being finalized for remote ad-hoc inspection and operations around the waste drums, and for this purpose we also designed and constructed a 1:1 prototype platform holding 4 phantom drums and equipped with sensors. Test results with radioactive sources showed very encouraging performance in terms of sensitivity, therefore we are planning to install a small demonstrator system around real radioactive waste drums quite soon. A possible final system will be distributed, fine-grained, robust, reliable, and based on low-cost components. An overview of the prototype system, along with the test procedures and results of real tests, will be shown at the conference.

Speaker: Dr Paolo Finocchiaro (INFN)

Slides Finocchiaro_Presentation.pdf

73 Principle and procedure for the baseline radiation risk assesment to the non human biota of tropical ecosystem: an elaborative approach at Domiasiat, India

Radiation risk assessment in the radio ecological world is a crucial and complex process. The uncertainty associated with this need to be sort out. A closed system of natural forest of 5 kms at the baseline level is taken into account. The varying radiation level was observed and the generic machine data were simulated and the detail scenario characterization has been conducted using ten premasters. The radiation (40K,232Th,238U )natural sink( Phudsyngkai) is identified and the reference species (garra lamta fish ) of the prevailing scenario has been identified. Interaction matrices has been drawned of the area. The BIOMASS model and FASSET has been implemented for authentication and it has been found that there is a great agreement between the prevailing natural radiation accumulation scenario and the machine based simulated data(14 species). On the ground of that total of 40 edible biota has been assessed for the risk.It has been concluded that the natural phenomena in the universe has the great agreement with the machine intelligence and could be equate and described in the complex linear equation of physics.

Speaker: Kumar Niranjan (North-Eastern HilL University Shillong Meghalaya)

10:40 coffee break

Session 6: Education

74 Fukushima nuclear catastrophe in Japan: its probable influences on the nuclear educational programs and global learnings about this catastrophe

The earthquakes and tsunami, which occurred in Japan on 11th of March 2011, damaged the Fukushima Nuclear Power Plants; resulting in a new global nuclear catastrophe, 25 years after Chernobyl. This is an extremely unlucky nuclear event, and will lead to very serious influences on the global nuclear programs including the educational programs on the field of nuclear science and technology. First, this will create good and new materials for anti-nuclear lobbies and they will use this opportunity for oppressing the political authorities to abandon governmental nuclear power programs. Of course, similar results were envisaged after Chernobyl, and only 25 years later, these could slightly be eliminated by the public; but, it seems that the elimination of the results of this second catastrophe will be much more difficult than they were for Chernobyl. Briefly, it can be concluded that the Fukushima catastrophe in Japan will support the concept of nuclear renaissance, which has been the heart of discussions on the scientific platform for several years. The basic principles of the concept of nuclear renaissance can be summarized as follows: 1) Nuclear energy production systems should eventually be non-proliferative of nuclear weapons, 2) Minimized long-lived wastes resulting from fuel cycle, 3) Good accordance with the environmentalist concepts, and so, easily accepted by the people. Now, the application of new safer technologies for construction of nuclear power plants should also be included into these basic principles of nuclear renaissance. In this contribution, the Fukushima nuclear catastrophe and its probable scientific, technological, social influences, and the global learnings will be criticized, and the precautions in the field of nuclear education will be proposed.

Speaker: Prof. Turan Ünak (INCS)

75 Physics dissemination through measurements of in-door radon

Many people associate the environmental radioactivity with the artificial radioactivity. The population knows few things about the natural radioactivity. From 2005 in the framework of both “Lauree Scientifiche” project (PLS), funded by Italian Education Minister, and a project sponsored by the National Institute of Nuclear Physics (INFN), scientific dissemination was promoted in the field of radioactivity. The projects have involved high school students, in particular in measurements of in-door radon. The collaborating students received introductory information explaining the radon concern and the survey procedures. At the same time, they received radon detectors with instructions and data sheets. Each student also received a questionnaire about the sampling site (address, building characteristics, room characteristics) and radon devices (device code, period and place of exposure, device position within the room, etc.). The overall monitoring, spanned over a period of five years from 2005 to 2010, was carried out using passive nuclear track detection technique, through the diglycol carbonate (C12H18O7) CR-39 In total, till now, we have placed about 500 detectors in dwellings and schools in 57 locations so as to cover the whole investigated region.. Detectors were placed once for each site for 90 days. The investigated area have shown medium-high indoor radon concentrations, higher than the Italian average of about 70 Bq/m3, with peaks of 500 Bq/m3 or more in buildings near active faults. Fortunately, only a small fraction of the measurements, about 1.5% of total, was found greater than EU and Italian action limits for houses and workplaces.

Speaker: Prof. Giuseppina Immè (Dipartimento di Fisica e Astronomia- Università di Catania, INFN Sezione di Catania)

Paper ID_173_3rd_INCC_IMME.doc ID_173_3rd_INCC_IMME.pdf

Session 7: Radiopharmaceutical Chemistry

76 Highlights of the 2010 Topical Meeting on Isotopes for Medicine and Industry

The 2010 Topical Meeting on Isotopes for Medicine and Industry, the second in a new series of embedded topical meeting of the American Nuclear Society (ANS), was held at the Society’s Winter Meeting, Las Vegas, NV, November 7 – 11, 2010. The meeting series reflects the continuing growth of radioisotopes for both medical and industrial applications and the rapidly expanding research at this forefront of nuclear science. As the recent global crisis in the supply of molybdenum-99 has generated public attention to the nuclear science, research and developments on alternate routes to supplement or replace current sources has intensified. Program goals in the USA have targeted 2013 for the establishment of a national supply chain. One day of the meeting focused on reactor-and accelerator-based production of molybdenum-99. This was followed by presentations on the development and production of other isotopes for medical research, diagnostics, and therapeutics. New research involving accelerator- cyclotron-produced isotopes was highlighted in the sessions; the broad activities involving alpha emitters were detailed. Contributions illustrated how the injection of new money and resources into isotope production research had already invigorated the field, excitingly demonstrated with the production of heavy elements from californium-252 over berkelium-249 to the creation of element 117. A panel discussion again pointed out recent success, but also remaining critical gaps, in the development and rejuvenation of academia and work force in this field.

Speaker: Dr Rolf Zeisler (NIST)

77 In vivo biodistribution of I-131 labeled bleomycin (BLM) and isomers (A2 and B2) on experimental animal models

BLM isolated from the fermentation products of Streptomyces verticillus in 1966 by Umezawa in Japan belongs to a family of structurally related small glycopeptides (1 kDa) that give rise to single-stranded DNA breaks and DNA double-strand breaks (DSBs) in a metal- and oxygen dependent manner1. The BLM used clinically is a mixture of three distinct isomers, A2 (the most abundant, 65 %), B2 (30 %), and DM, which is a deme thylated form of A2 (5 %). BLM is known to form complexes with a range of metals, some of which have been shown to exhibit tumor-localizing properties as demonstrated by radiotracer experiments, and subsequently by clinical imaging studies2. Furthermore, it has been proposed that BLM complexes may be useful for targeted radiotherapy using isotopes of indium or ruthenium 3. Although BLM catalyzes DNA cleavage with some degree of sequence specificity, it differs from conventional endonucleases by generating 3-phospho-glycolate blocked DNA ends. BLM is a potent cancer chemotherapeutic , but its clinical use is hampered by DNA damage-independent side effects including life-threatening pulmonary fibrosis. As these side effects are dose-dependent, rational combination of BLM with appropriate DNA repair inhibitors could conceivably be highly beneficial in the clinic1. Of the range of DNA lesions caused by BLM, DSBs are believed to be the most cytotoxic1, 4. In yeast, where even a single unrepaired DSB is eventually lethal. Telomeres consist of tandem hexanucleotide (TTAGGG)n repeats that cap the termini of eukaryotic chromosomes and play essential roles in maintenance of chromosomal stability and cell viability. The complex that is responsible for telomerase activity includes a reverse transcriptase that adds on telomeric repeats at the end of chromosomes using an RNA template. This enzyme is not active in most somatic cells but is active in most human tumors, and is, therefore, considered as being of high potential as a selective target for different anti-tumor strategies. One approach in the search for tumor-localizing radiopharmaceuticals of greater specificity and diagnostic accuracy is to investigate available chemotherapeutic drugs. This paper deals with BLM compounds, BLMs, and the attempts to radiolabel these compounds with an appropriate nuclide (such as 131I) and evaluate the usefulness of the resultant radiopharmaceutical for the diagnosis and management of malignant tumors using nuclear methods . In case of combination of the cytotoxicity of BLMs with high radiotoxicity of an appropriate radionuclide such as 125I or another Auger and/or a -emitting radionuclide, it is expected that very effective radiolabeled anti cancer drugs will be designed, which will have large potential applications in cancer therapy. Bleomycins (BLMs; BLM, A2, and B2) were labeled with 131I and radiopharmaceutical potentials were investigated using animal models in this study . Quality control procedures were carried out using thin layer radiochromatography (TLRC), high performance liquid chromatography (HPLC), and liquid chromatography (LC/MS/MS). Labeling yields of radiolabeled BLMs were found to be 90, 68, and 71 %, respectively. HPLC chromatograms were taken for BLM and cold iodinated BLM (127I-BLM). Five peaks were detected for BLM and three peaks for 127I-BLM in the HPLC studies. Two peaks belong to isomers of BLM. The isomers of BLM were purified with using HPLC. Biological activity of BLM was determined on male Albino Wistar rats by biodistribution and scintigraphic studies were performed for BLMs by using New Zelland rabbits. The biodistribution results of 131I-BLM showed high uptake in the stomach, the bladder, the prostate, the testicle, and the spinal cord in rats. Scintigraphic results on rabbits agrees with that of biodistributional studies on rats The scintigraphy of radiolabeled isomers (131I-A2 and 131I-B2) are similiarly found with that of 131I-BLM. REFERENCES 1) Chen J, Stubbe J (2005) Bleomycins: t owards beter therapeutics. Nat Rev Cancer 5:102 2) Kahn PC, Milunsky C, Dewanjee MK et al (1977) The place of 57Co-bleomycin scanning in the evaluation of tumors. Am J Roentgenol 129:267 3) Stern PH, Halpern SE, Hagan PL et al (1981) Cytotoxic activity, tumour accumulation and tissue distribution of Ruthenium-103-labelled bleomycin. J Natl Cancer Inst 66:807

Speaker: Dr Ugur Avcibasi (1)

78 Attempts to develop new synthesizing methods of 2-fluoro-2-deoxy-d-glucose radiolabelled with fluorine-18 (18F-FDG)

2-Fluoro-2-deoxy-D-glucose radiolabeled with Fluorine-18 (18F-FDG) is routinely used in nuclear medicine as a PET imaging radiopharmaceutical and nucleophilicly synthesised, in general, using mannose triflate as a precursor in the presence of Kryptofix 222TM as a catalyst in acetonitrile as a polar aprotic solvent, which involves the SN2 nucleophilic substitution reaction of 18F to 2-position of mannose triflate. The excess of 18F in the reaction medium has been removed by the use of a quaternary ammonium anion exchange Sep-Pak column, known QMA (QMA Sep-PakTM). This reaction process has been applied in routine 18F-FDG synthesis, using fully automatic commercial synthesizing modules. The total synthesizing time of 18F-FDG, using this procedure, requires about 30 - 45 min, which means that an important 18F activity, produced by cyclotron, is lost at the end of this synthesizing procedure. Of course, this raises the cost of 18F-FDG used for PET imaging. In this study, we have tried to develop two different easier and quicker ways for 18F-FDG synthesis, which will be able to be used in routine applications. The first is the isotopic exchange reaction between 18F ion and 19F of 2-fluoro-2-deoxy-D-glucose molecule was realised in water, at 95 ºC, for about 10 min. The second is Selectfluor TM, first tried to be labeled with 18F, then it was used to label 2-deoxy-D-glucose. In both cases, high radiolabeling yields were obtained.

Speaker: Mrs Gülcan Ünak (Ege University, Faculty of Science, Department of Biochemistry)

Paper ID_142_3_Gülcan_FDG_(Full_paper)_Last.doc ID_142_3_Gülcan_FDG__Full_paper__Last.pdf

79 Radiopharmacological studies: interaction of antidepressant fluoxetine with thyroid hormones metabolism

Using [I-125]-labeled iodothyronines as substrates, we applied our newly developed radiometric enzyme assays for iodothyronine deiodinases (IDs) of types 1, 2 and 3 (D1, D2 and D3), as well as the adapted radiometric assays for conjugating enzymes uridine 5’-diphospho-glucuronyltransferase (UDP-GT) and iodothyronine sulfotransferases (ST), in radiopharmacological studies of the interaction of an antidepressant drug fluoxetine (Fluox) with the metabolism of thyroid hormones (TH) in the rat. TH are supposed to control the activity of some neurotransmitters (e.g., serotonin), which are hypothetically involved in the pathogenesis of depressive illness. Inadequate activities of brain IDs could lead to local insufficient triiodothyronine concentration and might be, therefore, one of the pathogenic factors of depression. Conjugation of phenolic hydroxyl group of hydrophobic TH with UDP-glucuronic acid (catalyzed by UDP-GT) or with sulfate (catalyzed by ST) should lead to their increased water solubility and increased excretion in bile and/or urine and, therefore, to decreased TH plasma levels. The effects of subchronic administration (for 25 days) to Wistar rats of Fluox by itself (1.5 to 6 mg per animal per day) or 3,3´,5-triiodo-L-thyronine (T3) (10 micro g per animal per day) by itself or in combination with Fluox, on T3 production and degradation in the CNS and in different peripheral rat tissues were followed both, at the level of whole organism and at the molecular level. At the whole-body level, we found that administration of fluoxetine caused a slight decrease in serum total thyroxine (T4) levels, but produced only a negligible effect on T3 levels. The treatment of rats with supraphysiological amounts of T3 caused very marked decline of serum T4 levels, due to a feedback action of TH. Surprisingly, administration of Fluox together with supraphysiological amounts of T3 caused a distinctive fall of non-physiologically high concentrations of serum T3, which were reached by giving the animals the same amounts of T3 alone, to nearly normal levels. The elaborated radiometric assays for IDs, UDP-GT and ST were found usable for the assessment of enzymatic changes, at the molecular level. About two-fold higher UDP-GT activities were found in liver microsomes of the rats treated with Fluox in comparison with control rats. On the contrary, the enzyme activities of ST in the liver and kidney cytosolic fractions of the control and treated animals were found to be negligible and not influenced by the treatments. However, changes in IDs activities caused by the treatment of rats with Fluox alone, and especially with T3 by itself were much more pronounced and could be easily quantitated. This work was supported by the Academy of Sciences of the Czech Rep. (Research project No. AV0Z50110509), by the Ministry of Education of the Czech Rep. (Research project No. MSM0021622413), and by the Czech Science Foundation (Grant No. 304/08/0256).

Speaker: Dr Stanislav Pavelka (1Department of Radiometry, Institute of Physiology, Academy of Sciences of the Czech Republic, Prague and 2Central-European Technology Institute, Masaryk University, Brno, Czech Republic)

Companies

13:30 Lunch

Excursion 1: Erice and Segesta

Lectio Magistralis: at Segesta

80 Epistemiological consideration on Radiochemistry during its 115 years of development

In the first part of the presentation, some epistemological thoughts related to the connection between CHEMISTRY and RADIOCHEMISTRY are introduced. About 40 years before the birth of RADIOCHEMISTRY, a great debate was taking course in CHEMISTRY, concerning the essence itself of this new-born science, from the question of atomic and molecular weights to periodical properties of the elements and their compounds. Even if about further four decades before, the Avogrado’s principle, based on Gay-Lussac’s work, had been established, a great confusion existed. The first to have envisaged the potentiality of Avogadro’s principle and its correctness has been a young researcher, Stanislao Cannizzaro, born in Palermo (July 13 th 1826), who won the chair of chemistry in 1855, at the University of Genoa. In this University, he published in 1858 Sunto di un Corso di Filosofia Chimica, in which he gave the outmost value to Avogadro’s principle, by considering that if two gases, in the same temperature and pressure state, contain the same number of molecules, the ratio of their two volumes gives directly the ratio of their molecular weights (what we now call formula weights). During the presentation of these principles by Cannizzaro, four years after Avogado’s death, at the first International Congress of Chemistry of Karlsrule, in 1860, where also Dmitrij Ivanovič Mendeléev and Julius Lothar Meyer were present, the latter addressed to Cannizzaro a well known appreciation (you gave us back our sight). Interpretation of CHEMISTRY on the light of Periodic Table of elements was the necessary presupposition, 36 years later, to the birth of RADIOCHEMISTRY . Two cases of epistemological significance of pseudo-discoveries in the history of Radioactivity are then considered, the first one concerning Ausonium, Hesperium, and the discovery of nuclear fission, the second one connected to contamination by containers and to the eternal dream of alchemists, trying to convert lead or mercury into gold. Cameron and Ramsay (Le Radium, 1907, 4, 402) irradiated, by alpha particles, a very pure (or what they deemed so) aqueous solution, containing copper (II) nitrate and sulphate, and observed, by spectroscopy, the formation of traces of lithium, of neon, and of more considerable quantities of sodium. Their interpretation has been that radiochemical decomposition of copper (II) took place by this way. One year later, Marie Curie (M. Curie, E. Gleditsch, Le Radium, 1908, 5, 225) showed that it is extremely difficult, by operating in glass or quartz containers, to obtain distilled water rigorously free of lithium. By repeating the experiments of Cameron and Ramsay in platinum containers, no lithium nor sodium could be detected. A lesson for all radiochemists.

Speaker: Prof. Ignazio Renato Bellobono (LASA, Department of Physics, University of Milan, and B.I.T. srl, Milan, Italy)

Gala Dinner: at Segesta

Wednesday 21 September

Session 8: Nuclear Chemistry and Radiochemistry

Radiochemistry

81 Lead radioisotopes in the lower atmosphere associated with natural aerosols

The aerodynamic size distributions of radon decay product aerosols, i.e. 214Pb, 212Pb, and 210Pb were measured using low-pressure (LPI) as well as conventional low-volume 1-ACFM and high-volume (HVI) cascade impactors. The activity size distribution of 214Pb and 212Pb was largely associated with submicron aerosols in the accumulation mode (0.08 to 2.0 μm). The activity median aerodynamic diameter “AMAD” varied from 0.10 to 0.37 μm (average 0.16 μm) for 214Pb-aerosols and from 0.07 to 0.25 μm (average 0.12 μm) for 212Pb-aerosols. The geometric standard deviation, σg averaged 2.86 and 2.97, respectively. The AMAD of 210Pb-aerosols varied from 0.28 to 0.49 μm (average 0.37 μm) and the geometric standard deviation, σg varied from 1.6 to 2.1 (average 1.9). The activity size distribution of 214Pb-aerosols showed a small shift to larger particle sizes relative to 212Pb-aerosols. The larger median size of 214Pb-aerosols was attributed to α-recoil depletion of smaller aerosol particles following the decay of the aerosol-associated 218Po. Subsequent 214Pb condensation on all aerosol particles effectively enriches larger-sized aerosols. 212Pb does not undergo this recoil-driven redistribution. Even considering recoil following 214Po α-decay, the average 210Pb-labeled aerosol grows by a factor of two during its atmospheric lifetime. Early morning and afternoon measurements indicated that similar size associations of 214Pb occur, despite humidity differences and the potential for fresh particle production in the afternoon. In estimating lifetimes of radon decay product aerosols in ambient air, a mean residence time of about 8 days could be applied to aerosol particles in the lower atmosphere below precipitation cloud levels.

Speaker: Constantin Papastefanou (Aristotle University of Thessaloniki, Department of Physics, Atomic and Nuclear Physics Laboratory)

82 Marine sediments as a radioactive pollution repository in the world

During a time period little longer than 60 years, it has been created a radioactive pollution background over the natural one, which started in 1945 and it has been growing up since then, due to several nuclear tests, minor nuclear reactors failure and four major accidents: Wind Scale, Three Mile Island, Chernobyl and Fukushima. This radioactive polluting background can be easily detected through 137Cs fission product, which by the effect of wind, river currents and rain has been accumulated in marine sediments, mainly because sea represents about 80% of earth’s surface. Since energy demand has been growing up with no interruption during last two centuries, and nuclear energy seems to be the largest available source, it is very likely a great expansion of nuclear energy during XXI century. So, this paper presents results obtained in strategic points of the two large littorals in Mexico: Gulf and Pacific Ocean, as an attempt to establish there some figure to evaluate the present radioactive pollution. An adequate figure to do it, seems to be the quotient of activity per gram of 137Cs in marine sediments (Bq137Cs/g), divided by activity per gram of 40K natural radioactivity (Bq40K/g). When this result is multiplied by 100 the percentage of polluting radioactivity (137Cs) related to natural radioactivity (40K) is obtained. This percentage seems to be useful to evaluate the importance of radioactive pollution from 4 points of view: a)calculate the extent of already radioactive pollution present in the seas of world; b) avoid the panic in case of nuclear accidents, c) what will be the growing up rate in the future; d) if it is possible to keep one decreasing rate at same decaying rate of 137Cs (t1/2 = 30.07 years), since from 1945, starting time of radioactive pollution, it has decayed only about 2.2 half lives.

Speaker: Dr Manuel Navarrete (National University of Mexico)

Paper ID_38_Marine_sediments_Navarrete.doc ID_38_Marine_sediments_Navarrete.pdf

Slides Marine_sediments.pdf Marine_sediments.ppt

83 Correlation between the particle size distribution of radioactive aerozols and their half-lives derived from measurement of radioactive aerosols at a 120-GeV proton target station

High-energy proton beams traveling in air and beam sprays from the interaction of the beam with the target and related target station components produce radioactive aerosols in the target area. We report on the measurements of the radioactive aerosols produced in the Fermilab Anti-proton target station (AP0), where 120-GeV proton beam interacts with an Inconel target. Radioactive aerosols are produced either by direct activation by the beam and its secondaries and/or the subsequent attachment of the various radio-nuclides produced by other nuclear spallation reactions in the target, in the instruments around the target, air and other sources. The radio-nuclide composition of the radioactive aerosols and their correlation to the aerosol size distribution has not been studied previously. In order to control external and internal exposure of the workers to radioactive aerosols, it is important to understand the dynamics of radioactive aerosols in an accelerator target area. In this work, we separated radioactive aerosols which were collected from the AP0 target vault into several samples according to particulate size ranging from 0.056 to 10 micro-meters by using the “impactor method.” The particulate size distributions of radioactive aerosols associated with corresponding radio-nuclides were obtained by measuring the gamma rays of various radio-nuclides in each sample. The following fourteen radio-nuclides were identified in the aerosol samples: Na-24, Au-198, Sc-47, Au-196, V-48, Cr-51, Be-7, Co-56, Co-58, Sc-46, Co-57, Mn-54, Na-22 and Co-60 in the order of their half-lives. Consequently, it was found that the particle size distribution of radioactive aerosols is correlated with the half-lives of their constituent radio-nuclides. Based on the results, the dynamical and the formation mechanism of radioactive aerosols in the target area will be studied further.

Speaker: Dr Shun Sekimoto (Kyoto University Research Reactor Institute (KURRI))

84 Helium release from aged palladium tritide

In order to measure the helium release accurately, many methods including thermal desorption, P-V-T, mass spectrometric analyses and calorimetric measurements have been used. The article provides competitive measure methods of D-T isotope exchange, thermal desorption and aqua fortis dissolution to study helium release from PdTx. The methods of D-T isotope exchange and aqua fortis dissolution combined with mass spectrum and gas chromatogram analyses are original techniques. The helium release ratio of three aged samples were achieved by these methods. Palladium tritides at the initial tritium/palladium(T/Pd) atomic ratio of 0.65 were prepared by gaseous P-V-T method. Three samples were aged at room temperature for 604,1265 and 2168 days, respectively. The obtained results reveal that palladium tritides have the strong ability to retain 3He generated in their matrix, and 3He out gassed can not be obviously observed using D-T substitution and thermal desorption methods. In contrast, the helium release ratio of three samples (i.e., 1.94% of 604 days, 2.87% of 1265 days and 3.34% of 2168 days, respectively ), measured by aqua fortis dissolution method, indicate that more than 96.7% of 3He is held up in Pd and the 3He release ratio is increasing with aging time.

Speaker: Mr Zhi Zhang (China Academy of Engineering Physics)

85 Study of bioaccumulation and effect biomarker in mussels Perna perna (LINNAEUS, 1758: mollusca, bivalvia) from coastal regions of São Paulo State, Brazil

Studies on the coast of São Paulo identified contamination in water and sediment samples in the region of Santos, and bioaccumulation of contaminants in marine organisms. Based on these studies, there was a need to assess exposure and effects of trace elements in a sentinel organism in this region, by using the bivalve Perna perna. The mussels were evaluated for bioaccumulation of As, Co, Cr, Fe, Se and Zn by Instrumental Neutron Activation Analysis (INAA) and Cd, Pb and Hg were determined by Atomic Absorption Spectroscopy (AAS). Effect biomarker was assessed by evaluation of lysosomal membrane stability, using the Neutral Red assay (NR). The organisms were collected at two sites in São Paulo State coast (23º58´-23º39´S, 46º30´-45º25´W): Cocanha (mussel farm) beach in São Sebastião and Santos Bay (Itaipu and Palmas). Seasonally, the Perna perna were collected between September/08 and July/09 in each study site. Among the sites of collection of the mussels, it was verified that Cocanha was the site where the concentrations of the determined elements were higher in most cases. Concerning the seasonal variations, higher values of studied elements were found in wintertime. Opposite to winter, in the summer the highest NR retention (110±22, 76±25 e 100±25 minutes, Cocanha, Itaipu and Palmas, respectively) indicated less stress. NR results found in Santos were significantly higher than those found in Cocanha, being the highest stress rates attributed to Itaipu. Correlations between the trace elements studied and the integrity of lysosomal membrane are being studied.

Speaker: Dr Marina B. Agostini Vasconcellos (IPEN - CNEN/SP)

Slides Vasconcellos_128.pdf Vasconcellos_128.ppt

86 Validation of γ spectrometry technique to determine potassium in foodstuufs

The validity of a specific method should be demonstrated in laboratory experiments using samples or standards that are similar to unknown samples analyzed routinely. Aim of this work is the validation of γ the spectrometry technique to determine potassium in foodstuffs. It was evaluated the accuracy spiking a blank of calcium carbonate sigma ultra purity (potassium concentration lesser than 0.005%) with a known amount of pure Potassium chloride, the resulting mixture is measured in a γ-spectrometer with a high efficiency and low background 3"×3" NaI (Tl) scintillation detector surrounded by heavy shielding and coupled to a PC loaded with the Maestro Program. Obtained results are compared with the expected. Accuracy it also evaluated by comparison with concentration obtained by Atomic Absorption spectroscopy (AAS) in different types of samples (chili, corn meal “masa”, beans and tobacco) after acidic digestion, with a resulting r2 = 0.98. It was also evaluated the linearity, range, precision (reproducibility), and detection and quantification limits. Values obtained show that the used technique is acute, reproducible, and accessible to laboratories equipped with a low background scintillation detector.

Speaker: Trinidad Martinez (National University of Mexico)

Paper ID_80_MARTINEZ.doc ID_80_MARTINEZ.pdf

Slides MARTINEZ_ID-80.pdf

87 Fulvic acids, fertilizers first and then stimulants of vital functions in vertebrates

It is very well known from ancient times that fulvic acids present in Nature as a component of dead leaves and vegetables, are the active principle which promotes better crops , acting on mineral ions in soils by picking up them into plants tissues at higher concentrations. Tested in mice, by using radioactive labeled ions such as 32PO4---, 45Ca++, 59Fe+++ and 131I-, fulvic acids have demonstrated to stimulate the filtration of these ions from digestive tract to blood and then to urine by a factor larger than two. The following step on this research has been to find the effect caused by the presence in blood of electrolytes at higher concentrations, particularly viral infections resistance as a consequence of antibodies promotion.

Speaker: Dr Manuel Navarrete (Faculty of Chemistry, National University of Mexico)

Paper ID_37_Fulvic_acids_Navarrete.doc ID_37_Fulvic_acids_Navarrete.pdf

Slides Fulvic_acids.ppt

10:30 coffee break

Session 9: Radioecology and Geochemistry

88 Ultra low-level radionuclide analysis

The recent developments in ultra low-level radionuclide analyses include in the radiometrics sector availability of large volume HPGe detectors operating in underground laboratories very often with additional anti-cosmic shielding. In the mass spectrometry sector they include applications of Accelerator Mass Spectrometry (AMS), Inductively Coupled Plasma Mass Spectrometry (ICPMS) and Resonance Ionization Mass Spectrometry (RIMS) for analysis of long-lived radionuclides. Coupling of AMS with GC allowed transfer of analyses from bulk samples to compound specific isotope analyses of environmental samples. Very recent developments include a new ultra sensitive laser-based analytical technique, intracavity optogalvanic spectroscopy (ICOGS), allowing extremely high sensitivity for detection of tracers 14C, which is competing well with the AMS technique. Another example represents applications of ion trap mass spectrometry for ultra sensitive radionuclide analyses. These developments in both sectors did not only considerably decrease the detection limits for several radionuclides (up to several orders of magnitude), but they also enable to carry out investigations which were not feasible before either because of lack of sensitivity or because they required too large samples. Applications of radiometrics and mass spectrometry techniques in isotope oceanography, specifically on the distribution of 3H, 14C, 90Sr, 129I, 137Cs, 239Pu and 240Pu in the water column of the Pacific and Indian Oceans are presented and discussed in detail.

Speaker: Prof. Pavel Povinec (Comenius University of Bratislava)

89 Characterization of REE from NE Portugal using Instrumental Neutron Activation Analysis

The main objective of this study is the elemental characterization of geomaterial samples (“soils”, rañas and mother rocks), in terms of rare earth elements (REE), collected between 2007 and 2008, in the Morais Massif, (NE Mainland of Portugal) by using Instrumental Neutron Activation Analysis (INAA). The group of samples labeled “soil”, includes representative portions of the inorganic component (after C-removal) of the poor (immature) soil that rests over metaperidotite and metagabbro rocks belonging to the Morais Allochthonous Massif. Raña is a debris flow deposit typically composed of heterometric and (sub)angular pebbles of resistant materials (mostly quartzite, lidite, and milky-quartz masses) in a clay-supported matrix; relatively quietness periods of sedimentation between consecutive debris flow events are marked by discontinuous clay horizons variably enriched in silt or sand fractions. Samples (soil, mother rock and rañas) granulometric fractions lower than 63µm were separated and analyzed at the Portuguese Research Reactor, RPI. Chondrite normalization is done in order to obtain patterns indicators of REE anomalies. REE concentrations in soil samples are roughly half of the ones in the rañas.

Speaker: Dr Maria do Carmo Freitas (Instituto Tecnológico e Nuclear)

90 Application of the model of Cs-137 vertical migration for the assessment of sedimentation rates along the Bertioga Channel, São Paulo State, Brazil

Cs-137 is among the main isotopes produced in U-235 fission in nuclear explosions. It has a high fission yield, half-life of 30.17 years and decays to Ba-137 through β and γ emissions. As Cs-137 has a strong affinity to marine particulate matter, it tends to accumulate in sediments. This nuclide is largely used for estimating sedimentation rates, since historical dates of Cs-137 liberation in the environment (1963’s global fallout peak and 1986’s Chernobyl accident, for instance) can be identified in vertical profiles of radiocesium activity, and then be used to increase the precision of the models of sedimentation of unsupported Pb-210. However, Cs-137 behavior in sediments is complex due to numerous factors such as local sedimentary dynamics and vertical diffusion through interstitial water. Being so, radiocesium peaks cannot be used accurately for the purpose of sedimentation rates study without the application of a mathematical model which considers the main factors that cause these temporal modifications in Cs-137 vertical distribution. Bertioga Channel is part of the Santos-São Vicente Estuarine Complex, one of the economically most important regions in Brazil. It is a channel at the northeast portion of the complex, where three sediment cores where sampled for this study. Through the means of high-resolution gamma spectrometry, Cs-137 radioactivity was measured for the purpose of assessing local sedimentation rates using the model of vertical migration of Cs-137 proposed by LIGERO et al. (2005), chosen for considering the 1963 radiocesium initial input, not using excessive mathematical parameterizations, and being appropriate for coastal regions. The use of this model resulted in a mean sedimentation rate of 0.97 cm/yr.

Speaker: Paulo Ferreira (University of São Paulo)

91 Activity size distribution of radioactive Be-7 aerosols at different environments in Northern Italy

The activity size distributions of the natural radionuclide tracer 7Be were determined in different site places in Northern Italy in order to define any differences due to the different environments. In the frame of this work, three different environments where chosen, in an urban area (University of Milano), in a rural residential area (Ispra) and in Maqugnaga village at 1300 m height in Monte Rosa Mountain. Each sampling at three sampling stations was carried out simultaneously with a sampling at a reference station in an suburban-industrialised area (Segrate). For this case, two compatible aerosol cascade impactors were used. The aerodynamic size distributions were obtained by using two compatible 1-ACFM cascade impactors with efficient cutoff diameters (ECD) of 0.4, 0.7, 1.1, 2.1, 3.3, 4.7, 5.8, and 9 and acetate cellulose filters as collection substrates. The length of each collection period was 1 week. In order to study the influence of the meteorological conditions to the activity size distribution of 7Be aerosols, the three sampling campaigns at different environments were done during each season of the year.

Speaker: Prof. ALEXANDRA IOANNIDOU (ARISTOTLE UNIVERSITY OF THESSALONIKI, Physics Department, Nuclear Phys. and Elementary Particle Phys. Division)

92 Chemical composition of marine sediments in the Pacific Sea from Sinaloa to Jalisco in Mexico

Marine sediments from West coast of Mexico in the Pacific Sea from Sinaloa to Jalisco, Mexico were analyzed by the energy-dispersive X-ray fluorescence technique (EDXRF). 9 sediment samples were collected in May, 2010 at water depths between 55.5 and 1264 m with a box nucleate sampler type Reinneck. Sediments were dried and the total and separated fine fraction analyzed. Concentration and distribution of K, Ca, Ti Mn, Fe, Cu, Zn, Ga, Pb and Br were analyzed and compared with the reference values given by the Environmental Protection Agency (EPA) and Ontario Ministry of the Environment (MOE). In order to know the status of the elements in marine sediments, the enrichment factor and other index were calculated. It was also determined the pH, conductivity and total and organic carbon. Scanning electron microscopy and X-ray diffraction (XRD) show the predominant groups of compounds present in these marine sediments. As a Quality Control, Certified Reference Material was processed and analyzed at the same conditions.

Speaker: Prof. Trinidad Martinez (National University of Mexico)

Paper ID_89_Martinez.doc ID_89_Martinez.pdf

Slides MARTINEZ_T._ID_89.pdf

93 Chemical fractionation of radionuclides in submerged plants and sediments of the Yenisei River

The Yenisei River is contaminated with artificial radionuclides released by one of the Russian nuclear facilities (Mining-and-Chemical Combine), which has been producing weapons-grade plutonium since 1958. The submerged plants growing on radioactively contaminated river bottom sediments contain artificial radionuclides. Sequential extraction techniques are the most common method of studying radionuclide speciation in sediments and submerged plants. The aim of this study was to show that the sequential extraction approach can be successfully used to study remobilization of artificial radionuclides from sediments and submerged plants of the Yenisei River. Sediment and submerged plant samples were collected from the Yenisei River at different distances downstream of the Combine. Sequential extraction technique proposed by Tessier and modified by Klemt et al. (2002) was used to investigate sediment samples. Sequential extraction was performed in sediments that were in different states (wet, dried, and re-wetted). Some of the samples of sediments and the submerged plants were spiked with 241Am or 242Pu. The new sequential extraction scheme was used in this study for submerged plant samples, and the resulting fractions were exchangeable, adsorbed fractions, organics, and mineral residue. Sequential extraction performed on samples of the sediment cores collected near the Combine showed that the largest amounts of the radionuclides were extracted from such fractions as organics, oxides and hydroxides. We arranged radionuclides in the following sequence, showing their relative mobility in the upper layers of the cores: 90Sr ≈ 241Am ≈ 152Eu > 60Co >238U> 239,240Pu > 137Cs. The transuranic elements 239Np, 242Pu and 241Am were found in the intracellular fraction of the submerged plant biomass, and this suggested their active accumulation by the plants via the analog mechanism. Localization of radionuclides in the intracellular fraction of the biomass determines their further migration along trophic chains of the ecosystem and the subsequent toxic effect.

Speaker: Prof. Alexander Bolsunovsky (Institute of Biophysics SB Russian Academy of Sciences)

94 Micro-XRF and micro-EXAFS investigations of radionuclide sorption in Boda Siltstone Formation

Argillaceous rocks are being considered in many radioactive waste management programmes as suitable host rock formations for the deep geological disposal of radioactive waste. Clay minerals such as illite, smectite, illite/smectite mixed layers and kaolinite are important components in such rock types and can often make up 50 or more wt.% of the total mass. One of the most important characteristics of many clay minerals is their generally strong radionuclide retention properties. The rocks investigated were prepared from geochemically characterized cores from drillings in Boda Siltstone Formation, Hungary. The samples are albitic clay stones that represent the most significant constituent of Boda Siltstone Formation. Two polished 30-60 µm thick thin sections were prepared, and the thin sections were placed for 72 hours into a synthetic ground water solution representative for Boda Siltstone Formation with 0.1 mM Ni2+ or 1 mM Ni2+ added. After the treating period the samples were dried up by high pressure Ar gas. The micro-distribution and the local environment of nickel in the argillaceous rock samples were investigated applying micro x-ray fluorescence (micro-XRF) and micro extended x-ray absorption fine structure (micro-EXAFS) investigations at the micro-fluorescence Beamline L at HASYLAB (Hamburg, Germany). A polycapillary half-lens (X-ray Optical Systems) was employed for focusing a beam of 3 ×1.5 mm2 down to a spot size of 15 μm diameter. The EXAFS spectra were recorded in fluorescence mode at the K-absorption edge of Ni, recording the Ni-Kα fluorescent yield using an energy-dispersive silicon drift detector. A series of micro-EXAFS measurements were performed on the thin sections, at points of interest (POI) with varying Ni content. Micro-XRF elemental maps collected at an excitation energy of 17500 eV showed an anticorrelation with Ca and Fe, and a correlation with K-rich phases. This indicates that mainly clay rich minerals are responsible for the Ni uptake in the Boda formation. The precise identification of the particular nature of the clay minerals responsible for the sorption would need additional micro-XRD investigations. Using micro-EXAFS, the formation of precipitates and surface complexes could be clearly distinguished. The strong second peak in the radial structure functions (RSF) at R+ΔR = 2.7 Å indicates the formation of a precipitate from the Ni-containing synthetic ground water solution on the rock surface, and can mainly be attributed to Ni-Ni backscattering pairs. The micro-EXAFS spectra of a few POIs of the samples treated with 0.1 mM Ni2+, however, can be fitted without any Ni-Ni backscattering pair, indicating the formation of a surface complex. The obtained fitted structural parameters (5.3 Ni-O at 2.05 Å, 1 Ni-Al at 3.03 Å, and 2.1 Ni-Si at 3.3 Å) are consistent with Ni-uptake on edge sites of clay minerals. The research leading to these results has received funding from the Swiss-Hungarian Cooperation Programme through Project n° SH/7/2/11 and from the European Community's Seventh Framework Programme (FP7/2007-2013) under grant agreement n° 226716.

Speaker: Dr Szabina Torok (KFKI Atomic Energy Research Institute)

95 Traces of Fukushima accident in Southern Poland.

As a result of strong earthquake near Japan Islands followed by tsunami wave on 11 of March 2011 a serious damage caused by overheating occurred to reactors of the Fukushima Daiichi Nuclear Power Plant. Uncontrolled radioactive emission to the atmosphere started on 12 of March and was lasting for more than 2 weeks. Radioactive cloud migrated across Pacific, Northern America and came to Europe from northern-western direction The Institute of Nuclear Physics in Krakow operates high volume aerosol sampler MASS-500. The original flow rate of 500 m3/h is reduced to 250 m3/h when the charcoal gas double cartridge is added below the Petryanov filter. Collection of samples started on 21 of March and after detection of 131I on 24 of March the cartridges and filters were changed every day till 11 of April, later the measurements were continued in larger periods. Filters and charcoal were analyzes on low background gamma spectrometer with HPGe detectors. The fallout was collected in two weeks intervals using 2.2 m2 area collector and few persons (Polish citizens) who come back from Japan were analyzed using whole body spectrometer equipped with two HPGe detectors. The presence of 131I, 132I, 129mTe, 132Te, 134Cs,136Cs and 137Cs was established in air filters. Measurable concentrations of cesium appeared three days later that those from iodine. The maximum activity in Krakow for 131I, 134Cs and 137Cs was observed on 28 and 29 March and it was 6 mBq/m3 , 0.6 mBq/m3 and 0.4 mBq/m3 for 131I, 134Cs and 137Cs, respectively. Average activity ratio for 134Cs to 137Cs was 1.11. The ratio between activity in aerosol fraction 131I to gas fraction was changing with time, being almost equal to 1 in the maximum activity it was then increasing to less than 5 in mid-April. In thyroids of Polish citizens who came back from Japan up to 28012 Bq of 131I were found. The estimation of effective dose equivalent (including not well known details of inhalation scenario) yields in about 10 Sv. A search for Pu, Am and Cm isotopes was performed to two sets of filters and to fallout samples. Since the analyses are not finished at the time of writing the abstract all results will be presented during the conference.

Speaker: Mr Kamil Brudecki (The Henryk Niewodniczanski Institute of Nuclear Physics, Polish Academy of Sciences,)

96 The dynamics of radioactive aerosols in the atmosphere of Moscow by the "Fukushima" nuclear power plant accident.

As a result of the accident at the “Fukushima” nuclear power plant, caused by an earthquake, there were releases of radioactive substances into the environment. To date, many countries reported on the flow of radioactive aerosols from Japan and the radioactive contamination of the environment, as well as food (1,2,3,4). Intake of radioactive aerosols in Moscow was registered at radiation monitoring stations of SIA “Radon”, "March 23, 2011. Using powerful air sampler led to the identification of radioactive aerosols in the atmospheric surface layer of Moscow: 131I, 132Te, 134Cs, 136Cs and 137Cs. Maximum volume concentration of these radionuclides were, respectively: 2,7•10-3 Bq/m3, 7,7•10-5 Bq/m3, 4,8•10-4 Bq/m3, 2,1•10-5Bq/m3, 6,8•10-4Bq/m3. Simultaneously, it was determined the ratio of volume activity concentration of the aerosol form of iodine to the volume activity concentration in gaseous form, which amounted to 3,3 ± 0,2. In addition, it was determined the ratio of activity concentration of 137Cs and 134Cs. This ratio is equal to 1,4 ± 0,2. Method of stack filters have produced baseline data for evaluating the dispersion characteristics of radioactive aerosols originating from Fukushima accident in Moscow surface air. References 1.http://en.wikipedia.org/wiki/radiation effects from Fukushima 1 nuclear accidents 2.http://www.syracuse/com/news/index/ssf/2011/03/fucushima fallout reaches euro.html 3.http://news.scotsman.com/scotland/Radiation fallout detected in Glasgow.6742690.jp 4. http://www. the totalcollapse.com/independent-french-radiation-commision-warns-europe

Speaker: Dr Sergey Gordeev (Scientific and Industrial Association "Radon")

13:30 Lunch

Excursion 2: at Monreale and Palermo

Dinner: at Mondello

Thursday 22 September

Session 10: Nuclear Chemistry and Radiochemistry

97 Revisiting the ultimate condition for applicability of k0-NAA: the constancy of neutron flux parameters during irradiation

In the development of k0-standardized neutron activation analysis (k0-NAA), a number of criteria were identified and worked out both theoretically and practically, that should be taken into account for achieving reliable analysis results. Among these, the ones most frequently considered and reported upon in publications dealing with the implementation and the application of k0-NAA are: i) the choice of accurate input nuclear data (k0-factors; Q0-values; effective resonance energies; half lives etc.), ii) the characterization of the irradiation facility (f - thermal to epithermal neutron flux ratio; alpha - epithermal neutron flux shape factor), and iii) the calibration of the Ge-detector (detection efficiency; peak-to-total ratio). However, a hardly mentioned and indeed often overlooked criterium, which was nevertheless identified to be the ultimate condition and restriction for the applicability of k0-NAA, is the constancy of the neutron flux parameters during irradiation. Therefore, in the present paper this topic is again brought to the attention, not only dealing with theoretical considerations but also considering practical aspects and giving examples taken from the daily practice.

Speaker: Dr Frans De Corte ((em.) UGent and FWO-VL, Neerstraat 20, B-9921 Vinderhoute, Belgium)

98 The half-lives of Y-90m and Ru-97

Accurate nuclear measurements depend on well-controlled experimental and numerical work, both in the execution of daily measurements and in the creation and evaluation of fundamental constants needed to connect the laboratory with the International System of Units. It cannot always be assumed that tabulated data are sufficiently accurate for all routine work. The k0 Nuclear Data Committee has identified a number of radionuclides whose half-lives are not adequately known for accurate neutron activation analysis, as judged by disagreements between published evaluations. We have applied gamma-ray spectrometry and least-squares methods developed for other nuclides to redetermine the decay constants of 90mY and 97Ru. Irradiated samples of each pure element were counted continually through several half-lives, acquiring up to 100 spectra with good statistics. Photopeaks from each nuclide were evaluated with a fixed-boundary integration routine, and each resulting data point corrected for rate-related losses before fitting to an exponential function by a nonlinear least-squares procedure. Preliminary values are 3.205 ± 0.005 h for 90mY and 2.84 ± 0.01 d for 97Ru, where the uncertainty is the standard deviation of the mean of several determinations. Although by chi-squared criteria the fits to the decay curves were very good and the uncertainty of the resulting half-lives an order of magnitude smaller than the published discrepancy, care is necessary before assigning a best value with a totally defensible uncertainty to the overall data set.

Speaker: Dr Richard Lindstrom (National Institute of Standards and Technology)

Paper ID_36_Halflife_paper_A4_Lindstrom.doc ID_36_Halflife_paper_A4_Lindstrom.pdf

Slides ID_36_Halflife_talk_Lindstrom.pdf

99 Conversion of I2 in ionic forms on the composite materials "Fizkhimin"TM in water coolant at nuclear power plants

It is known that the activity of radioactive iodine in the water coolant increases dramatically during the shutdown of reactors on the Russian working WWER- or RBMK-type NPPs. For example, the radioactivity of 131I in the water coolant increased 30 to 200 times during the shutdown of the reactor on the RBMK-type NPP such as the Leningrad and Smolensk NPPs. One of the reasons of this activity rise is that during the shutdown of a reactor the temperature of the fuel inside the fuel elements drops, which results in the reduction of the fuel volume and the appearance of free space inside the fuel elements. Simultaneously, water from the coolant penetrates into the fuel elements through defects in the fuel cladding and dissolves radioactive iodine and caesium accumulated in the gap between the fuel and cladding during normal operation of NPP. The dissolved radioactive iodine and caesium go as ions to the water coolant. Due to different redox reactions in a water coolant radioactive iodine can be present as ionic (I-, IO3-) and molecular (I2) species. Furthermore, the radiation-induced destruction of the ion-exchange resins can lead to the formation of organic species (such as CH3I) in a water coolant. At the same time the content of radioactive iodine in the gas phase increases by more than an order of magnitude, because molecular and organic forms of radioactive iodine make a major contribution to the pollution of the gas phase since their factors of distribution between the water and gas phases are several orders of magnitude higher than those for ionic forms. We suggest that an analogous increase in the radioactive iodine content in the water coolant and gas phase during the shutdown can occur also in the currently working and new developed NPPs using a water coolant. To decrease the radionuclide content in the water coolant, cation- and anion-exchange resins are usually used during a normal operation of NPPs. For example, cation-exchange resin KU-2 and anion-exchange resin AV-18 were used on the Russian NPPs for coolant decontamination. However, anion-exchange resins can absorb effectively only ionic forms of radioactive iodine and possibly I2 as anion I3-. We studied the sorption of CH3131I and I2 on an AV-18 ion-exchange resin from the water coolant which takes places on the some of the Russian WWER-type NPPs. It was found that the AV-18 anion-exchange resin can absorbs I2 and CH3131I from the solution. After 2 h of contact between liquid and solid phases, I2 absorption was about 70%, whereas the CH3131I absorption was only about 30.0%. Anion-exchange resin AV-18 effectively absorbs I2 (more than 99%) from this water coolant of a WWER-type NPP only after 24 h of contact between the liquid phase and the resin. In this case the distribution factors Кd for I2 were higher than 103 cm3/g, whereas the distribution factors Кd for CH3131I were lower than 200 cm3/g. Because of a low rate of sorption of I2 and CH3I the anion-exchanged resin AV-18 could not effectively and quickly localize these forms of radioactive iodine from the water coolant. These findings made it apparent that a new more effective material to absorb molecular and organic iodine from water solutions was required, and it was desirable to employ materials used in working NPPs to coolant decontamination. In our experiments, we used ion-exchange resin KU-2, which we modified to obtain sorptive materials. The materials IPCE-C1 and IPCE-C2 with about 8.0 and 5.5 wt.% of Cu), and also IPCE-CS with about 10.1 wt.% of Cu and Ag were obtained and used for our bath experiments. For these materials, we studied sorption of different forms of radioactive iodine (131I-, 131IО3-, CH3131I) and I2 from water coolant which takes places on the some of the Russian WWER-type NPPs.. Preliminary experiments showed that the non-modified cation-exchange resin KU-2 has a low sorption capacity for CH3131I and I2 in the studied solution: the distribution factors are not higher than 5.0 cm3/g at V/m = 100. At the same time under similar experimental conditions the distribution factors Кd for I2 for all developed materials are higher than 103 cm3/g. The distribution factors Кd for ionic forms change from 20.0 to 150 cm3/g, whereas for the organic form, they are not more than 11.0 cm3/g. As follows from the data on I2 sorption kinetics on our developed materials and anion-exchanged resin AV-18, during 15 min of contact between the solid and liquid phase practically full I2 absorption (more than 99.0%) takes place on the modified resin KU-2 vs. 50% on the resin AV-18. As above-mentioned, the 99% absorption of I2 on anion-exchange resin AV-18 can be achieved only after 24 h. Unfortunately, the developed materials have low efficiency for CH3131I in the studied solutions. So, our findings allow us to conclude that using a combination of our developed materials and anion-exchanged resins such as AV-18 would allow to more effectively decontaminate the water coolant from ionic and molecular forms of radioactive iodine and partially organic form in working and new developed NPPs. Also note that the application of the new materials will not require changes in either the designs of NPPs or the reactor’s water coolant decontamination sites and will allow to bring down the load on the iodine filters during the shutdown and refueling of a reactor, as well as normal operation of the NPPs. Work is supported by Council about grants of the President of the Russian Federation for the state support of leading scientific schools of the Russian Federation (grant SS-6692.2010.3).

Speaker: Prof. Sergey Kulyukhin (Institute of Physical Chemistry and Electrochemistry RAS)

Paper

• ID_1_Kulyukhin.doc
• ID_1-Kulyukhin.pdf
• ID_1_Kulyukhin.pdf

Slides

• Presentation_ID_1-Kulyukhin-new.pdf
• Presentation_ID_1-Kulyukhin-new.ppt
• Presentation_ID_1-Kulyukhin.pdf
• Presentation_ID_1-Kulyukhin.ppt

100 2-Secure facilities for Egyptian Nuclear weapons

- Egyptian Nuclear weapons states have developed dedicated safe and secure facilities for nuclear warhead and bombs assembly and disassembly operations .These facilities are critical elements of material nuclear weapons infrastructures .Their broad operational responsibilities include the production of new warheads, the dismantlement of retired warheads ,warhead modernization and refurbishment, stockpile surveillance and component testing ,production of trainers, and modification of stockpiled warheads for flight-testing purposes such as an operation involving replacement of fissile components with inert materials and telemetry systems .The facility is defined as a nuclear warhead assembly/disassembly plant ,If it conducts the operations of assembly/disassembly of nuclear explosive packages (NEP),an assembly containing high explosive (HE),components and fissile materials, and/or final mechanical assembly of warheads (Bombs). As such operations involve staging and handling of fissile materials components and assemblies including NEPs and fully assembled warheads , The facility's states could be defined as "Shutdown" or "Converted" .If it no longer works with intact nuclear weapons or subassemblies containing fissile materials. In this second paper ,I will complete my first paper that published the SPIE2010 and I discuss and present the main secure facilities for Egyptian nuclear warheads and bombs and the major monitoring options for former warhead assembly/disassembly facilities that could be used in combination with each other ,and show some cases of nuclear forensic investigations.

Speaker: Prof. Prof.Dr.Mr.Ashraf Elsayed Mohamed Mohamed (Institute for Nuclear Materials)

101 Selective reduction of actinyl ions based on electrocatalysis using platinized glassy carbon fiber column electrode

Some actinide ions such as U, Np and Pu exist stably as trivalent to hexavalent ions in an acidic solution. The adjustment of the oxidation state of these ions to a desired one is inevitable for the efficient chemical separation or the precise determination of them, since chemical reactions such as liquid-liquid distribution and complex formation with ligands depend strongly on the oxidation state of the ions. Electrode reaction of tetravalent (An4+) and pentavalent (AnO2+) ions couples, which accompanying formation or cleavage of An-O bond, is generally irreversible and requires a large overpotential. For this reason, selective control of oxidation state of actinide ions by electrolysis is difficult. The authors have studied redox mechanisms of actinide ions, and recently clarified that electrocatalytic reaction at Pt electrode can decrease overpotential of reduction of NpO2+. In the present study, platinized carbon fiber electrodes were examined as a working electrode of the flow electrolysis in order to develop a rapid electrolytic method for controlling oxidation state of actinide ions. The column electrode is composed of a working electrode of a bundle of very thin glassy carbon fibers packed tightly in a cylindrical electrolytic diaphragm of porous glass, and it enables quantitative and rapid electrolysis in a flow system. Flow electrolysis was performed by passing a solution containing actinide ions through a column electrode. For reduction of NpO2+, overpotential of the reaction was reduced, and successive reductions of NpO2+ to Np4+ and that of Np4+ to Np3+ were observed. This result indicates that the selective preparation of Np4+ by electrolysis can be achieved successfully. For reduction of Pu, overpotential of reduction of PuO2+ was also mitigated, and hence reduction of PuO22+ to Pu3+proceeded selectively at much positive potential. In contrast, the reduction of UO22+ to U4+ was little affected by working electrode materials.

Speaker: Dr Yoshihiro Kitatsuji (Japan Atomic Energy Agency)

Slides 55_YKitatsuji.pdf

102 Behavior of thorium on poly(vinyl pyrrolidone) grafted with citric acid prepared using gamma radiation

The behavior of thorium on poly(vinyl pyrrolidone) grafted with citric acid in HCl-media has been investigated using -spectrometry. Various factors has been studied such as: treatment of PVP, concentration of grafted acid, concentration of HCl, concentration of thorium, and contact time. The results have shown that thorium is adsorbed on the resins in high acid concentration (5-7 mol/l HCl) by grafting ratios of about 2%, provided that the prepared resin has been treated with hydrochloric acid or sodium hydroxide. The time needed to reach the adsorption equilibrium was relatively short and the effect of the concentration of grafted acid is relatively strong. The resins were prepared by irradiation of ternary mixtures of PVP/Citric acid /water by gamma rays at a dose of 25 kGy in air and at ambient temperature. The maximum swelling and the gelation % of the prepared resins were investigated. Swelling and gelation decrease with increasing the concentration of grafting acid. The decrease of the maximum swelling is due to increased hydrogen bonding between the carboxyl groups of the bonded/ trapped citric molecules and the hydroxyl groups of the polymer. The decrease in the gel fraction can be explained by the presence of the acid that leads to other reactions in the mixture and not preferably to building cross links between the polymer chains.

Speaker: Dr Oussama Alhassanieh (Atomic Energy Commission of Syria AECS)

103 Chemiluminescence of luminol - sodium hydroxide system using hemin as catalyst

Abstract The chemiluminescence (CL) emission spectra of luminol in aqueous sodium hydroxide [Na(OH)2] system has been recorded in presence of hemin using various oxidants. Hydrogen peroxide, potassium ferricyanide, potassium permangnate, and potassium persulphate are the various oxidants used. There is no emission of light observed when potassium persulphate has been used as an oxidant. The microphotometric traces of CL emission spectra are re-plotted on a linear wavelength scale. On the basis of CL emission spectra resolultion the mechanism has been explained. A 460 nm band appears for potassium ferricyanide when used as oxidant while two emission bands are observed for hydrogen peroxide and potassium permanganate when used. The mechanism has been explained by decomposition of transannular peroxide to form excited 3-APA which has been responsible for the intense CL emission in presence of hemin.

Speaker: Dr Neeta Lala (Universiti Malaysia Pahang)

Paper ID_196_3rd_INCC_-_13_Feb_12__FULL_PAPER_(Neeta_Lala).docx ID_196_3rd_INCC_-_13_Feb_12__FULL_PAPER__Neeta_Lala_.pdf

10:30 coffee break

Session 11: Radioanalytical Chemistry and Nanoparticles

104 Automated and rapid determination of radionculides for emergency analysis, radioecology investigation and characterization of decommissioning waste

With the increasing threat of potential nuclear terrorism and radiological accidents, establishment of a rapid reaction system under nuclear emergency preparedness is an urgent requirement for reducing the health risk to the public. Rapid determination of radionuclides in large number of biological and environmental samples is a key and crucial step in the emergency process and determines the whole reaction time. With increasing numbers of nuclear facilities being closed in recent years and from now on, a considerable decommissioning work is needed, and characterization of various wastes from decommissioning is required for evaluation of the radioactivity inventory in various materials. In the radioecological investigation, a large number of environmental and biological samples need to be analysed to obtain a better estimation of the environmental risk. All these work requires to accurate determination of various radionculides. Except for the gamma radionuclides, the traditional analytical methods for radionuclides normally take a few days to weeks for one analysis; this makes the emergency reaction impossible in one day, and impossible to analyse a large number of sample from decommissioning work and radioecological investigation. In recent years, considerable efforts have been focused on the development of automated and rapid analytical methods. In our laboratory, automated analytical systems have been established by exploiting flow/sequential injection approach, using chromatographic separation concept, combined with rapid measurement of radionculides using ICP-MS. A number of analytical methods have been developed to determine 99Tc, 237Np, and isotopes of Pu, U and Th in biological, environmental and nuclear waste samples. This work aims to summarize these automated and rapid analytical methods for the determination of various radionculides.

Speaker: Prof. Xiaolin Hou (Risø National Laboratory for Sustainable Energy, Technical University of Denmark)

105 Multi-dimensional chromatographic separations of actinides

Many radioisotopes are released in the environment from our use of the nuclear energy. Among these, actinides are a health concern due to their long environmental persistence and the risk associated with internal dosimetry. The simultaneous analysis of actinides (i.e. Th, U, Np, Pu and Am) is labour-intensive because 1) they are found at ultra trace levels, 2) are difficult to dissolve, 3) have sometimes instable valence and 4) interfere together and with the matrix constituents. A new partly-automated extraction chromatography (EXC) separation methodology was developed to overcome those issues. Environmental samples are dissolved by fusion in 2M hydrochloric acid in order to ensure complete dissolution of refractory species. Using TEVA and DGA resins, multidimensional chromatography based on valence and media adjustment was performed in order to separate each radioelement, thus limiting the presence of isobaric and molecular interferences during the analysis. On-line valence adjustment is performed to facilitate elution or improve retention of some actinides. Eluted fractions, containing the separated actinides, are measured by either alpha spectrometry and/or inductively coupled plasma mass spectrometry (ICP-MS), providing complementary isotopic information. Because of the specificity of each type of instrumentation, effect of matrix constituents were assessed. This approach has great potential for automation of emergency responses methodologies, improving sample throughput while minimizing human error and the necessity to be performed by highly-qualified personnel. Initial automation efforts will be presented.

Speaker: Prof. Dominic Lariviere (Université Laval)

106 Optimization of Sequential Separation of U, Th, Pb, and lanthanides for ultra-trace analysis

Abundance and isotopic ratios of trace uranium (U), thorium (Th), lead (Pb) and lanthanides in environmental samples play a key role to investigate features of the samples. The analytical data may give information on origin of the sample, dating of mineral formation, history on mineralization, and age determination of nuclear materials. Abundance and isotopic ratios of an element of interest are generally measured with high resolution inductively-coupled plasma mass spectrometers (HR ICP-MS). In most environmental samples such as rocks, soils, and airborne dusts, trace U, Th, Pb, and lanthanides are contained with major elements such as Na, K and Fe. These major elements and the polyatomic ions which originated from the co-existing elements affect accuracy of analytical results measured by ICP-MS [1, 2]. The analytes, therefore, should be separated from the interfering elements. Chemical separations are good solution for accurate analyses, but the procedures are generally complicated and time-consuming. The authors developed the technique for sequential separation of U, Th, Pb, and the lanthanides using a single anion-exchange column (resin: Muromac 1x8, particle size: 100-200 mesh, column size: 5.5 mm in diameter, 42 mm in height) and mixed media consisting of hydrochloric acid, nitric acid, acetic acid, and hydrofluoric acid [3]. With a single anion-exchange column, sequential separation of 50 ng each of U, Th, Pb, and the lanthanides in an ICP-MS calibration solution was successfully carried out. Using a mixture of acetic acid and other mineral acids (hydrochloric acid and/or nitric acid) enabled complete separation of the analytes. The absorption of the elements of interest on the column was enhanced in the mixture of acetic acid compared with simple hydrochloric acid and nitric acid media. Alkali metals, alkali earth metals, and Fe were eliminated from U, Th, Pb, and the lanthanides. The recovery yields of the elements of interest were more than 95%. This sequential separation technique was applied to an automatic system. The eluents were pressurized by compressed air, and injected into an anion-exchange column. The separation of elements of interest was optimized for several parameters including particle size, column length, and eluent flow rate. The elements of interest were completely separated within 6 hours. The peak resolution of elution curves were improved by using the pressurized separation system. This work was supported by financial aids from the Ministry of Education, Culture, Sports, Science and Technology (MEXT) of Japan (Scientific Research (C): Grand No. 22550143). [1] Magara, M., Sakakibara, T., Kurosawa, S., Takahashi, M., Sakurai, S., Hanzawa, Y., Esaka, F., Watanabe, K. and Usuda, S., J. Nucl. Sci. Technol. 39, 308-311 (2002). [2] Magara, M., Sakakibara, T., Kurosawa, S., Takahashi, M., Sakurai, S., Hanzawa, Y., Esaka, F., Watanabe, K. and Usuda, S., J. Aanl. At. Spectrom. 17, 1157-1160 (2002). [3] Miyamoto, Y., Yasuda, K., Magara, M., Kimura, T. and Usuda, S., J. Nucl. Radiochem. Sci. 10,7-12 (2009).

Speaker: Dr Yutaka MIYAMOTO (JAEA (Japan Atomic Energy Agency))

107 Detection of ultratrace amounts of Np-237 with resonance ionization mass spectrometry (RIMS)

Long-lived isotopes of the actinides are the major contributors to the radiotoxicity of spent nuclear fuel after a storage time of 1000 years. Especially Np-237 is considered as a potential hazard to the environment because of its long half-life of 2.14 million years and high mobility in aquatic systems. Since the concentration of Np-237 expected in case of a leakage of a nuclear waste repository is less than 0.1 nM, migration studies require very sensitive methods for the determination of Np-237. Resonance ionization mass spectrometry (RIMS) has proven to be a powerful method for ultratrace analysis of actinides. Therefore, a RIMS method for the detection of Np-237 has been developed by us and will be presented. In RIMS, an atomic beam of Np-237 is evaporated from a heated filament, and the atoms are ionized with radiation from three tuneable lasers. The wavelengths of the lasers match subsequent optical transitions of the element. The laser ions are detected by a time-of-flight mass spectrometer. Since the involved optical transitions are unique for Np-237, this kind of ionization process is element specific. Thus, mass spectra free of isobaric interferences and with a very low background can be recorded. Since only few high lying energy levels of Np-237 suitable for excitation and ionization were known, extensive spectroscopic studies were carried out [1]. With the identified energy levels, several three-step excitations schemes have been developed. Currently, an overall detection efficiency for Np-237 of 2E-6 has be obtained by RIMS. [1] S. Raeder, N. Stöbener, T. Gottwald, G. Passler, T. Reich, N. Trautmann, K. Wendt: Determination of a three-step excitation and ionization scheme for resonance ionization and ultratrace analysis of Np-237, Spectrochim. Acta B, in press, doi:10.1016/j.sab.2011.02.002

Speaker: Mr Nils Stoebener (University of Mainz - Institute of Nuclear Chemistry)

108 Radiological study of transport and processing of naturally occurring radioactive materials.

Background: Recently the European Commission is recasting the Euratom Basic Safety Standards (BSS) in order to further limit the exposure of the public and workers to radioactivity. The new BSS is expected in 2015 and contains a broad list of industries, processing Naturally Occurring Radioactive Material (NORM), that will become subject to more strict regulation. The list contains, among others, zirconium-, thorium-, and titanium-mineral processing plants, phosphate-ore industries and oil and gas extraction facilities. In addition the new BSS provides additional regulation for the incorporation of residues of NORM (fly ash, phosphogypsum, phosphorus/tin/copper slag, red mud, …) in building materials. Materials&methods: A large scale radiological study of the container traffic in the port of Antwerp was conducted by means of portal monitors. Geometry corrected in-situ measurements were performed on materials in industrial processes with LaBr(Ce) and Na(Tl) probes. These results were compared with analysis of samples by means of a Ge detector. Results: (1) A database of the NORM traffic through the port of Antwerp (2008 – 2010) was constructed. (2) Though measurements in the port of Antwerp and at companies a new user-friendly method for the determination of the activity concentration was developed. The determined activity concentrations were compared with the limits set by the BSS. The results obtained with several types of probes in industrial setting are compared. (3) In case-studies dose on workers was assessed. (4) The initial results of the measurement on building materials are shown. Outlook: A new strategy for the treatment of NORM contaminated waste will be investigated. IAF and NuTeC organize the 4th EAN-NORM workshop in Hasselt, Belgium (Nov 29th – Dec 1st 2011). The workshop focuses on transportation of NORM, measurements strategies and building materials (http://www.ean-norm.net/). Acknowledgement: Funding for the research projects is provide by the ministry of the Flemish community, EFRO and LRM.

Speaker: Wouter Schroeyers (CMK (UHasselt) and NuTeC (XIOS Hogeschool Limburg))

Slides NuTeC_3eINCC_slides.pdf

13:00 Lunch

INCS General Assembly

16:00 coffee break

Session 12: Radiopharmarmaceutical Chemistry

109 Paving the way to personalized medicine: production of some theragnostic radionuclides at Brookhaven National Laboratory

This presentation will introduce a relatively novel paradigm that involves specific individual radionuclides or radionuclide pairs that have emissions that allow pre-therapy low-dose imaging plus higher-dose therapy in the same patient. We have made an attempt to sort out and organize a number of such theragnostic radionuclides and radionuclide pairs that may potentially bring us closer to the age-long dream of personalized medicine for performing tailored low-dose molecular imaging (SPECT/CT or PET/CT) to provide the necessary pre-therapy information on biodistribution, dosimetry, the limiting or critical organ or tissue, and the maximum tolerated dose (MTD), etc. If the imaging results then warrant it, it would be possible to perform higher-dose targeted molecular therapy in in the same patient with the same radiopharmaceutical. A major problem that remains yet to be fully resolved is the lack of availability, in sufficient quantities, of a majority of the best candidate theragnostic radionuclides in a no-carrier-added (NCA) form. A brief description of the recently developed new or modified methods at BNL for the production of a number of theragnostic radionuclides, whose nuclear, physical, and chemical characteristics seem to show great promise for personalized cancer therapy will be described.

Speaker: Suresh C. Srivastava (Medical Department, Brookhaven National Laboratory, Upton, New York 11973, U.S.A.)

110 Cyclotron production of Sc-44 - new radionuclide for PET technique

Objectives: Two isotopes of scandium, 47Sc and 44Sc, are perspective radionuclides respectively for radiotherapy and diagnostic imaging. 47Sc decays with the half-life of 3.35 days and maximum β- energy of 600 keV. It also emits low-energy γ-radiation (Eγ = 159 keV) suitable for simultaneous imaging. The other scandium radionuclide, 44Sc (t1/2 = 3.92h) is an ideal β+-emitter in PET diagnosis. It can be used as an alternative to 68Ga, because 44Sc has longer half-life and forms stable radiobioconjugates with a structure similar to 90Y and 177Lu, that is important in planning radionuclide therapy [1]. 44Sc can be obtained as a daughter radionuclide of long-lived 44Ti (t1/2 = 60.4y) from 44Ti/44Sc generator or can be produced by nuclear reaction 44Ca(p, n)44Sc in small cyclotrons. The aim of our work was to find optimal parameters for 44CaCO3 target irradiation in order to maximize the production of 44Sc with minimal impurities of the longer half-life 44mSc and to develop a simple chemical procedure for separation of 44Sc from the calcium target. Methods: In the present work, we used highly enriched 44CaCO3 (Isoflex, Russia). The irradiations have been performed with the Scanditronix MC 40 Cyclotron of the Joint Research Centre (Ispra, Italy). Designed aluminum capsules were filled with 2 mg of dry 44CaCO3 powder, inserted into a water cooled target holder and were irradiated at different beam proton energies. For each of the irradiation, a Ti foil was used as a proton beam energy monitor. The activity of the different samples were measured with high resolution -ray spectrometry. Longer-lived 46Sc was used instead of 44Sc in the separation procedure. The CaCO3 target was dissolved in 1 ml of 0.1 M HCl. Then, the solution was passed through a column filled with iminodiacetic resin Chelex-100. After adsorption of 46Sc the column was washed with 30 ml of 0.01 M HCl and the effluent containing enriched calcium was collected for further irradiations. The 46Sc was quantitatively eluted with 1 M HCl in the second 0.5 ml fraction. Results: The 44CaCO3 target was irradiated by protons in the range of 5.5-23MeV. The analysis of several irradiations indicate that the amount of 44Sc reached the maximum, with the lowest production (0.16%) of 44mSc impurity in the energy range of 9-10MeV. 46Sc was separated from the target on iminodiacetic resin with efficiency of more than 95%, eluted in volume of 0.5 ml. The recovery of the calcium target is nearly quantitative. The level of Ca2+ in 46Sc fraction is less than3 g/ml. Conclusions: The low-energy irradiation of 44Ca gives opportunity to produce Ci level activities of 44Sc. The separation process proposed of 44Sc from the target is simple and fast. The 44Sc obtained can be used instead of 68Ga in PET diagnosis and planning radionuclide receptor therapy.. Research Support: This work was carried out as a part of the project of the Ministry of Science and Higher Education of Poland DWM/N166/COST/2007 and COST Action D38. References: [1] A.Majkowska, A.Bilewicz, (2011), J.Inorg.Biochem. 105, 313–320.

Speaker: Prof. Aleksander Bilewicz (Institute of Nuclear Chemistry and Technology)

111 99mTc(N)-DBODC(5) from cardiology to oncology: preliminary in vitro study

99mTc(N)-DBODC(5) is a lipophilic cationic mixed-compound currently under clinical investigation as potential myocardial imaging agent. The findings that this complex accumulates in mitochondrial structures through a mechanism mediated by the negative mitochondrial membrane potential, and that the rapid efflux of 99mTc(N)-DBODC(5) from non-target tissues seems correlated to the Pgp/MDR-Pgp transport function opens the possibility to extend the clinical applications of this class of complexes to tumor imaging and non invasive multidrug resistance studies. Standing on this ground, the kinetic of uptake at 4 and 37 °C of 99mTc(N)-DBODC(5) was evaluated in vitro in suitable human cancer cell lines, and in the corresponding sub-lines, before and after MDR-modulator treatment, using 99mTc-Sestamibi as reference. Results from this study clearly indicated that: ì) the uptake of both 99mTc(N)-DBODC(5) and 99mTc-Sestamibi was correlated to metabolic activity of the cells. In fact, low temperature inhibited the cellular uptake of both 99mTc-tracers indicating that there was no binding to the cell membranes or to the hydrophobic regions of the cell membrane protein. ìì) The cellular accumulation is correlated to the level of Pgp/MRP expression, in fact an enhancement of uptake in resistant cells was observed after treatment with a MDR inhibitor/modulator, indicating the selective blockade of Pgp/MPR prevents efflux of the tracers. This study give a preliminary indication on the applicability of 99mTc(N)-DBODC(5) to tumour imaging and to the detection of MDR-mediate drug resistance in human cancer.

Speaker: Prof. Alessandro Dolmella (University of Padova, Italy)

Poster Section 2

112 [188Re(N)(cys~)(PNP)]+/0 mixed ligand compounds as models for the development of target specific agents

An efficient procedure for the preparation of [188Re(N)(PNP)]-based complexes is reported. The radiochemical yield (RCY) of the compounds was optimized considering reaction parameters such as: nature of nitrido nitrogen donors, reaction times and pH. The chemical identity of 188Re-agents was established by HPLC comparison with the corresponding well characterized cold Re-compounds. The stability of the [188Re(N)(PNP)]-complexes toward transchelation with GSH and degradation by serum enzymes was assessed. The clearance of selected radiolabeled agents from normal tissues was evaluated in rats. [188Re(N)(cys~)(PNP)]+/0 asymmetrical compounds were prepared in aqueous solution from perrhenate using a multistep procedure based on the preliminary formation of the labile 188ReIIIEDTA species which easily undergo to oxidation/ligand exchange reaction to afford in presence of DTCZ the [188ReV≡N]2+ core. The final compounds were obtained by adding to the [188ReV≡N]int 2+ the two bidentate ligands. However, a relative high amount of cys~ ligand was required to obtain a quantitative RCY. The complexes were stable toward reoxidation to perrhenate and ligand exchange reactions. In vivo studies showed a rapid distribution and elimination of the complexes from the body. No specific uptakes in radiation sensitive tissues/organs were detected. A positive correlation of the distribution of the complexes estimated with biodistribution studies (%ID) and with micro-SPECT semiquantification imaging analysis (SUV) was observed. The low labeling efficiency limits but not excludes the possibility to apply [188Re(N)(PNP)]-technology to the preparation of target specific radiotherapeutical agents.

Speaker: Prof. Alessandro Dolmella (University of Padova)

113 A new radiofluorination method of select fluor as a new and effective F-18 fluorinating reagent

1-(Chloromethyl)-4-fluoro-1,4-diazoniabicyclo[2.2.2]octane ditetrafluoroborate is known as SelectfluorTM (Sigma-Aldrich Cas no. 140681-55-6) and is a widely used as an electrophilic fluorinating agent for different kinds of organic compounds. Contrarily, it was not used for 18F fluorination processes, but recently a research team at Oxford University in the UK has tried to label 1-(Chloromethyl)-4-fluoro-1,4-diazoniabicyclo[2.2.2]octane bis(triflate) with 18F as another form of SelectfluorTM. For this procedure, direct fluorination of 1-chloro-methyl-4-aza-1-azoniabicyclo [2.2.2] octanetriflate (accessible in two steps from triethylenediamine, TEDA) was performed in dry CH3CN at -10 °C with fluorine (10 % F2 in N2). In this study, 1-(Chloromethyl)-4-fluoro-1,4-diazoniabicyclo[2.2.2]octane ditetrafluoroborate form of SelectfluorTM was radiolabeled with 18F. For this radiolabeling procedure 250 mL saturated solution of SelectfluorTM in water was prepared and 250 µCi (9.25 MBq) 18F was added. Then, this mixture was evaporated in a water bath up to dryness in about 10 min. The dried mater was again dissolved in 50 µL water and the samples taken from this solution were analyzed using TLC technique. The TLC analyses have showed that SelectfluorTM was radiofluorinated with 18F with about 95 % radiofluorination yield. This radiofluorinated SelectfluorTM with 18F was successfully used for 18F fluorination of 2-fluoro-2-deoxy-D-glucose and insulin. Thus, a new and effective 18F fluorinating agent has been introduced as a widely usable agent in 18F fluorination chemistry.

Speaker: Mrs Gülcan Ünak (Ege University, Faculty of Science, Department of Biochemistry, Bornova, Izmir 35100, Turkey)

Paper ID_164_7_Gülcan_Selectfluor_(Full_paper)2.doc ID_164_7_Gülcan_Selectfluor__Full_paper_2.pdf

114 A recoil method for Be-7 radiolabelling of nanoparticles

Nanoparticles (NPs) have been used in a variety of applications for many decades, without specific attention being given to safety issues that may be due to their small dimensions. Examples of products in which NPs are used are suncreams, printer toners, car tyres, and pigments. In recent years, the rapid growth of the field of nanotechnology has seen surge in the number of different types of NPs used in industrial processes and consumer products. This has given rise to concern as to whether materials in the form of nanoparticles can be considered equivalent to the same material in coarser powder form for safety assessments. Safety studies require knowledge of the behaviour of NPs, and this in turn requires a method of reliably detecting them and assessing their concentrations. Radiolabelling represents one of the most sensitive and quantitative techniques for this, but also poses several practical difficulties. For safety studies, ideally the material produced and supplied by industry should be used. However radiotracers cannot easily be incorporated into the industrial process, so post-synthesis radiolabelling needs to be used. While surface attachment of radiolabels, via chelating molecules, is an option, this also poses questions regarding changed NP properties due to the surface modifications, and also the stability of the NP-radiolabel construct in different environments. Alternatively, neutron or ion-beam irradiation can be used, under carefully controlled conditions, to directly activate most industrial NPs, but some types cannot be activated to useful levels due to the absence of a suitable reaction product under irradiation. More specifically silica and alumina cannot be directly activated to useful activity levels, and carbon-based NPs (nanotubes, etc.) need a proton beam of more than about 32 MeV to achieve reasonable activity levels. We describe here a recoil method for 7Be labelling of such NPs, based on the 7Li(p,n) 7Be reaction. The NPs of interest are mixed with a powder of an appropriate Li-containing compound, and the mixture is irradiated with a proton beam of approximately 5 to 3 MeV on target. The 7Be radionuclides recoil as a result of momentum transfer and energy release during the nuclear reaction process, and a fraction of these are implanted into the NPs to be labelled. The Li containing compound may then be “washed” off the NPs, leaving stably 7Be radiolabelled material. Theoretical considerations on various aspects, including recoil range and thermal effects, are presented, and initial experimental results are given for recoil labelling of SiO2, Al2O3, carbon nanotubes, carbon “buckyballs” and nanodiamonds.

Speaker: Ms Izabela Cydzik (Joint Research Centre European Commission, IHCP)

115 Adsorption of Cs(I) on Densely Crosslinked Poly(sodium methacrylate) from Aqueous Solutions

Toxic or radioactive metals cause progressive or irreversible renal injury and in acute cases, may lead to kidney failure and dead (1-3). Nuclear technologies have provided a better quality of different fields of life. However, this leads to accumulation of substantial amounts of radioactive wastes or waste solutions and the radionuclide 137Cs is produced in high yield during the fission processes. It is potentially very hazardous nuclide due to its long half-life (t1/2=30.17 years) and is a very radiocontaminant having high solubility in aqueous media (1, 4-6). Therefore there is a need for removal/separation of toxic or radionuclide metal ions from aqueous waste solutions or wastes by using organic or inorganic adsorbents. Many separation and preconcentration techniques such as chemical precipitation, ion-exchange, solvent extraction and sorption on the solid have been developed to remove metal ions from aqueous waste solutions. Nowadays, there is an increasing effort for removing toxic or radionuclide contaminants from aqueous waste solutions or wastes by using various polymeric adsorbents (6-10). It is also known that the use of polymeric adsorbents has advantages for controlling adsorption capacity and may present selective adsorption of metal ions from waste solutions. In this study, a crosslinked copolymer has been proposed to remove Cs(I) ions from aqueous solutions. For this purpose, the crosslinked copolymer of ethylene glycol dimethacrylate(EGDM) and methacrylic acid (MA) containing 25% of MA as weight percentage was synthesized by using benzoyl peroxide (BPO)-N,N-dimethyl aniline (DMA) initiator system at room temperature. The available groups of carboxylic acid in the crosslinked copolymer were converted to the groups of sodium methacrylate using 2 N NaOH solution. The adsorption behavior of cesium ions on the densely crosslinked poly(sodium methacrylate) from aqueous solutions were investigated by the technique of ICP-MS measurements. Batch adsorption method was used to analyze the Cs(I) adsorption as a function of parameters such as the amount of adsorbent, contact time, pH of solution, initial Cs(I) concentration and temperature. Adsorption data obtained from experimental results have been tested for a number of kinetic and isotherm equations. The constants in adsorption isotherm and kinetic equations have been determined. The adsorption free energy has been calculated by using D-R isotherm to adsorption data. References 1. Sheha R. R., Metwally E., J. Hazard. Mater., 143 (2007) 354-361. 2. Özeroglu C., Keçeli G., Radiochim. Acta, 97 (2009) 709-717. 3. Mellah A., Chegrouche S., Barkat M., J. Colloid and Interface Sci., 296 (2006) 434-441. 4. Cho Y., Komarneni S., Appl. Clay Sci., 43 (2009) 401-407. 5. Başçetin E., Haznedaroğlu H., Erkol A.Y., Appl. Radiat. Isotop., 59 (2003) 5-9. 6. Zhang Z., Xu X., Yan Y., Desalination, 263 (2010) 97-106. 7. Özeroğlu C., Keçeli G., Radiochim. Acta, 95 (2007) 459-466. 8. Maheswari M.A., Subramanian M.S., React. Funct. Polym., 66 (2006) 1452-1464. 9. Özeroğlu C., Keçeli G., J. Radioanal. Nucl. Chem., 268 (2006) 211-219. 10. Choi S-H., Nho Y.C., Radiat. Physics and Chem., 57 (2000) 187-193

Speaker: Dr Cemal OZEROGLU (Istanbul University Faculty of Engineering Department of Chemistry 34320 Avcilar-Istanbul/TURKEY)

116 Americium and samarium determination in aqueous solutions after separation by cation-exchange

Tasoula Kiliari, Ioannis Pashalidis* Department of Chemistry, University of Cyprus, P.O. Box 20537, Cy-1678 Nicosia *E-mail: pspasch@ucy.ac.cy ABSTRACT The concentration of trivalent americium and samarium in aqueous samples has been determined by means of alpha-radiometry and UV-Vis photometry, respectively, after chemical separation and pre-concentration of the elements by cation-exchange using Chelex-100 resin. Method calibration was performed using americium (Am-241) and samarium standard solutions and resulted in a high chemical recovery for cation-exchange. Regarding, the effect of physicochemical parameters (e.g. pH, salinity, competitive cations and colloidal species) on the separation recovery of the trivalent elements from aqueous solutions by cation-exchange has also been investigated. The investigation was performed to evaluate the applicability of cation-exchange as separation and pre-concentration method prior to the quantitative analysis of trivalent f-elements in water samples, and has shown that the method could be successfully applied to waters with relatively low dissolved solid content. Keywords: trivalent f-elements; determination; cation-exchange; composition; chemical recovery

Speaker: Mrs Tasoula Kiliari (University of Cyprus)

Paper Americium_and_Samarium_Determination_in_Aqueous_Solutions_after_Separation_by_Cation-Exchange_-3rd_INCC_paper.doc Americium_and_Samarium_Determination_in_Aqueous_Solutions_after_Separation_by_Cation-Exchange_-3rd_INCC_paper.pdf

Poster T.Kiliari_44.pdf T.Kiliari_44.pptx

117 An automated production of Cu-64 on 18/9 MeV cyclotron

The reaction route 64Ni(p,n)64Cu is very popular for the preparation of 64Cu because its entrance channel is accessible at low energies and yield of reaction is quite high. However, a high price of the enriched 64Ni is a disadvantage of this reaction path; hence, preparation of a chemically pure nickel targets for the production of 64Cu using COSTIS (Compact Solid Target Irradiation System) is of a great research interest. Composition of electrolytic bath and electrochemical process conditions on the quality of nickel films deposited on 2 mm thick gold disc targets was investigated. Chemical purity of the electrodeposited nickel was measured by the Auger electron spectroscopy and the surface quality of targets was studied microscopically (SEM). A SRIM program was used for a thickness target calculation. COSTIS target station was installed at the end of the external beam line of the IBA Cyclone 18/9 cyclotron, and the irradiation surface of target was optimized. The target station has been equipped by a Nb window foil in the front of the target to degrade the beam energy to an optimal value. 64Cu production rate for 100 mg 64Ni of 99.09 % purity (ISOFLEX) on gold target was 104 MBq/µAh. Chemical separation of 64Cu from 64Ni was achieved by anion exchange chromatography method using 6 M HCl as elution solution. An automated separation module for isolation of 64Cu equipped with PLC SIMATIC S7-1200 controller has been developed. The quality of 64Cu was checked by gamma spectrometry and chemical purity (64Ni) was determined by ICP-MS.

Speaker: Prof. Pavol Rajec (BIONT, Comenius University)

118 Ascertainment of changes in thyroid hormones metabolism in white adipose tissue by radiometric enzyme assays

Thyroid hormones (TH) play important roles in the development and function of both, brown and white adipose tissue. However, data about the local conversion of TH in adipocytes are still scarce. With the aid of our newly developed radiometric enzyme assay, we measured changes in the activity of the type 3 iodothyronine deiodinase (D3) in several depots of murine white adipose tissue (WAT) during the development of dietary obesity in the experimental animals. D3 is the key enzyme in the metabolism of TH, catalyzing the conversion of biologically most active 3,5,3'-triiodo-L-thyronine (T3) and also of prohormone thyroxine (T4) into inactive metabolites, 3,3'-diiodothyronine (T2) and 3,3‘,5‘-triiodothyronine (reverse T3), respectively. Changes in the metabolism of TH during the development of dietary obesity were followed in male C57BL/6J mice. At four weeks of age, the animals were randomly assigned to a standard low-fat (LF) diet or a special high-fat (HF) diet and maintained on these diets for two weeks before analysis. In addition to radiometric determination of D3 activities at the molecular level, changes in the thyroid status of the animals at the whole-body level were monitored. Serum total T3 and T4 levels were determined using commercial RIA kits. Moreover, several morphological parameters were followed, among others the assessment of cellularity of WAT depots by fluorimetric determination of tissue DNA concentration. Compared to LF diet, HF-feeding resulted in a significantly higher fat depots weight: epididymal fat depots (366 ± 19 vs. 242 ± 13 mg in LF controls), dorsolumbar subcutaneous fat (200 ± 7 vs. 143 ± 4 mg). Cellularity of the subcutaneous fat of HF group, assessed as DNA content, was higher (304 ± 52 vs. 215 ± 13 micro g DNA/depot) while no difference was found in epididymal fat. Plasma levels of total TH were significantly elevated in mice fed the HF diet: T3 (1.30 ± 0.03 vs. 0.96 ± 0.03 nmol/L), T4 (41.6 ± 1.1 vs. 36.9 ± 0.8 nmol/L). D3 activity was significantly enhanced in the subcutaneous fat of the HF-mice (142 ± 20 vs. 85 ± 12 fmol T2/h/mg protein in LF controls) but not so much in epididymal fat. In conclusion, we found that the development of HF diet-induced obesity in mice was associated with an enhancement of D3 activity in WAT. This work was supported by the Academy of Sciences of the Czech Rep. (Research project No. AV0Z50110509), by the Ministry of Education of the Czech Rep. (Research project No. MSM0021622413), and by the Czech Science Foundation (Grant No. 304/08/0256).

Speaker: Dr Stanislav Pavelka (1Department of Radiometry, Institute of Physiology, Academy of Sciences of the Czech Republic, Prague and 2Central-European Technology Institute, Masaryk University, Brno, Czech Republic)

Poster

• poster
• Sicily114-P-WAT-D1+D3.pdf
• Sicily114-P-WAT-D1+D3.pdf

119 Automated fusion methodology for the rapid dissolution of airborne actinides

Micro-wave acid dissolution is an effective and commonly used technique to dissolve environmental samples. However, this technique has several issues, including its low sample throughput, its limited ability to deal with samples containing high organic content such as biological tissues, and its incomplete digestion yields for refractory compounds like actinides oxides. An improved methodology based on the dissolution by automated fusion followed by extraction chromatography for the detection and quantification of actinides in environmental samples has been developed. A fusion protocol for the complete ashing and dissolution of various samples was optimized. Cross-contamination between samples was studied and results shown no evidence of such process even without washing the crucibles between samples. The automated fusion unit also improved repeatability in sample preparation over conventional muffle furnace fusion. Instrumental issues originating from the presence of high lithium concentration in the digestate after lithium metaborate fusion were also investigated. Consequently, a method using extraction chromatography (EXC) has been developed to remove lithium and the environmental matrix while keeping all the actinides in solution. The overall method was tested on several environmental reference materials of different composition. This methodology was applied to the monitoring of uranium airborne particulate in the province of Québec. Results obtained from microwave digestion and automated fusion were compared with respect to precision, detection and rapidity.

Speaker: Prof. Dominic Lariviere (Université Laval)

120 Basic information about nuclear power energy to mexican citizens

Mexico remains a country of vast territory; therefore, with increasing and more urgent energy demands, we consider indispensable the acceptance of Nuclear Power as a clean energy source, and thus fight back among the population the misconceptions which lead to irrational rejection as a viable alternative in the development of our country. As background, we will point out some facts made by ourselves, and others made by government or educational institutions, both nationally and internationally. We can present as precedent the inclusion in a secondary education book of a project for the preservation of monuments, which originally was designed as a typical research project in Nuclear Chemistry. There have also been bibliographic studies to verify that currently very few books talk about the nuclear problem in specialized texts of General Chemistry. In December 2010, an international seminar was organized with the participation of researchers from Toshiba Co., representatives from the National Institute for Nuclear Research, the Engineering Academy, the Mexican Nuclear Society, the World Energy Council, the Energy Regulatory Committee and the Ministry of Energy, etc. We believe that the most important issue of these projects is to raise public awareness about the safety in the use of nuclear energy as a clean and necessary source to enable a country's sustainable development. Mexico has only one nuclear plant with two reactors at Laguna Verde, in Veracruz, whereas most developed countries smaller in size have as many as six or seven of them favorable for their development, such as Finland and France. It is necessary that the population in general is educated and, therefore, accepts the installation of new plants to revitalize the economy and the development of any growing country.

Speaker: Dr Manuel Navarrete (UNAM)

Paper ID_116_BASIC_INFORMATION_FULL_Navarrete.doc ID_116_BASIC_INFORMATION_FULL_Navarrete.pdf

Poster BASIC_INFORMATION.ppt

121 Calibration protocol of Fricke-gel layers for absolute dose measurements in radiotherapy.

The continuous development of new approaches and skills in modern radiotherapy, aimed to achieve highly conformal dose volumes, have made heavy demands on dosimetry methodology development. The three-dimensional treatment planning computerized systems, adopted in the clinical praxis for radiation therapy, require dosimetry methods capable of reliable 3D dose measurements in order to ensure that the calculated values agree with the delivered dose distributions, also in complex treatments. The good tissue equivalence of Fricke-Gel Layer Dosimeters, which consist in a diluted water solution, and the independence of their response on photon energy in the range of interest for radiotherapy, constitute valuable characteristics for appropriate in-phantom dosimetry. Moreover, their layer geometry has allowed the development of a calibration procedure that enable achieving a precision within 3% in absolute dose measurements. The calibration is performed irradiating the dosimeter at a uniform and precisely known dose, in order to get a calibration matrix that must be used, with pixel-to-pixel manipulation, to obtain the dose image. A study of the trend in time of dosimeter response after successive exposures was carried out to draw up two protocols allowing to perform calibration and measurement or on the same day or on two subsequent days. As a final protocol, if calibration and measurement are carried out on the same day, it has been established to perform an irradiation of all dosimeters at 4 Gy, a second irradiation at 5 Gy for calibration purpose and the measurement with the calibrated dosimeters. On the opposite, if the measurement is performed the day after calibration, it has been established to perform only one irradiation of all dosimeters at 5 Gy and the measurement the day after. The comparison of the in-phantom experimental results with the values calculated by the treatment planning system has showed the validity of the proposed protocol.

Speaker: Dr Roberta Guilizzoni (Università degli Studi di Milano)

122 Characterisation of a Cu selective resin for use in the production of Cu isotopes for medical purpose

Cu isotopes (e.g. Cu-64) increasingly find use in radiopharmaceutical applications; accordingly fast, reliable and easily automatable methods for the production of these isotopes are of great interest. A Cu selective extraction chromatographic resin (CU Resin, TrisKem International) developed for the fast and selective separation of Cu was characterized and a method for the separation of Cu from different target materials was developed. The characterization of the resin included the determination of k’ values of Cu, Ni, Zn and other potentially interfering elements and impurities for varying acids and pH values as well as the influence of macro amounts of Ni and Zn on the extraction of Cu. Based on the obtained results, a method for the separation of Cu, and its purification from irradiated Ni or Zn targets was developed and tested on simulated Ni and Zn targets, and on an irradiated natural Ni target. Cu yields and decontamination factors for potential interferents have been determined, and the conversion of the Cu eluate to lower acid concentrations studied for the developed method. It could be shown that the CU resin has high selectivity over the tested interferents and that Cu can be recovered with high yield and purity in a small volume of 8M HCl within few minutes separation time.

Speaker: A. Bombard (Triskem International)

123 Characterization of radioactive waste from a PET cyclotron facility by gamma spectroscopy

Introduction Most of the waste generated at a cyclotron/PET facility presents high radioactivity created by target irradiation. The main sources of this waste are foils, spent targets, materials produced during accelerator maintenance, chemicals used in the separation of radioisotopes from the target materials and for labelling of radiopharmaceuticals. Usually, these materials are collected on-site in a designated area and then transferred to authorized companies for disposal from the site. Aim of this study is the qualitative and quantitative characterization of waste coming from labelling tracer procedures and cyclotron maintenance. Materials and Methods The PET centre at San Raffaele Scientific Institute is equipped with two cyclotrons, IBA Cyclone (18 MeV) and CTI Eclipse (11 MeV). 18F and 11C are produced by means of proton bombardment on [18O]H2O with Ag/Nb target (Havar/Ti foils) and on [14N]N2 + 1% O2 with Al target (Al foil), respectively. Typical productions for 18F and 11C, with a 60 min irradiation at a beam current of 50 microampere (18F) and 35 microampere (11C), range from 50 to 55 GBq. Two types of waste were considered: solid produced from cyclotron maintenance (cotton applicator, paper, gloves, QMA cartridges, stripper target) and liquid from FDG synthesis. Five solid and three liquid Al containers (10 kg for solid and 5 kg for liquid waste), relative to seven months, were analyzed. Spectroscopic measurements were performed using an High-Purity Germanium detector with 18% relative efficiency and 0.14% energy resolution at 1332 keV. Energy and efficiency calibrations were performed with 152Eu and 133Ba certified sources. A 1 ml sample of liquid waste was measured in the same geometry used for efficiency calibration. The total activity was then obtained by normalizing for the weight of the liquid in the container. In order to allow direct measurements of activity in the container (both liquid and solid waste), such total activity value was then used to determine correction factors for the container geometry (in the energy range from 50 to 2000 keV) at 15 cm far from the detector. In order to assess our technique, one Al solid container was sent for spectroscopic analysis to an ISO 9001 certified laboratory (LENA – University of Pavia). Results Analysis of waste of a typical solid container, filled in 2/3 months, showed the presence of relatively long-lived radionuclides: 7Be, 22Na, 48V, 51Cr, 54Mn, 56Co, 57Co, 58Co, 60Co, 65Zn, 95mTc, 108mAg, 109Cd, 110mAg, 182Ta. Measured activities ranged from 0.2 to 6.5 MBq. The main contribution arose from 7Be (6 MBq, T1/2=53.12 days), 58Co (3.5 MBq, T1/2=70.86 days) and 65Zn (2 MBq, T1/2=244.26 days). Liquid waste data confirmed the presence of 22Na, 51Cr, 54Mn, 56Co, 57Co, 58Co, 65Zn and their total activities ranged from 0.3 to 5 MBq. Spectroscopic analysis carried out by LENA confirmed same nuclides and activities within 20% of difference. The kind of radionuclides found in this study are inherent with the targets and foils employed for proton irradiation. In particular 7Be is likely obtained from the nuclear reaction 7Li(p,n)7Be, 48V from 48Ti(p,n)48V, all Co isotopes from natFe(p,x)Co or natNi(p,x)Co, 54Mn from 54Fe(p,n)54Mn, 65Zn from 65Cu(p,n)65Zn and 109Cd from 109Ag(p,n)109Cd. Short-lived contaminants could not be detected from our delayed measurements. Conclusion The presence of long-lived contaminants in the activated parts of accelerators (e.g. targets, foils) have been well established. Our results indicate that attention should also be given on waste produced during maintenance procedures and that long-lived radionuclides are present in the residuals of tracer synthesis, even if yield of radionuclides can vary depending on several factor such as cross section, exposure time, beam current and type of maintenance. Due to the presence of long-lived radionuclides, waste in-house storage is not useful and, therefore, waste disposal by authorized companies is recommended. However, procedures for waste minimization should be set-up as part of the safety assessment, to control potential risks and to reduce operating costs.

Speaker: Dr Ignazio Vilardi (Nuclear Medicine Department, Multimedica Scientific Institute, Sesto San Giovanni (MI), Italy)

124 Compare plutonium isotopes activity in humans bones on the area where only global fallout was present and the area where Global and Chernobyl fallouts ware present.

Plutonium isotopes are present in investigated samples mainly as a result of nuclear weapons tests in last century and Chernobyl disaster. In human body plutonium is accumulated mainly in liver and bones and main exposure pathway is inhalation. Bone tissue samples were obtained during routine surgeries – the replacement if knee or hip joints by implants. Patients belong to general population, not exposed in any special way to radioactive contamination. Surgeries were conducted in a V Military Hospital in Kraków in Southern Poland and in a general Hospital in Bielsk Podlaski in Northeastern Poland,. The patients originated from vicinity of hospital thus Pu from only Global Fallout was expected in case of Kraków and mixed Global and Chernobyl fallout was expected in case of Bielsk Podlaski. Studies got an approval of council for ethics in medical research. Sampels were ashen in 600oC for two days. The ashes were gently soaked of 6M HCl. Precipitation of calcium oxalates at pH=3 was completed to obtain transuranic fractions. Calcium oxalates was dissolved of 1M HNO3. The oxidation state of Pu was adjusted to +4 using hydrazine and NaNO2 and after conversion into 8M HNO3, the fractions were passed through Dowex-1x8. Pu remains in the column was eluted using 50 ml. of 0.1M HF - 0.1M HCl. Alpha spectrometric Pu sources were prepared directly in the solutions using NdF3 method. In Southern Poland in investigation involved 23 people, 9 men, 11 women, and 3 person who did not specified their gender in a quastionary. . The youngest patient was 56, while the oldest 88 years old. The obtained values for 239+240Pu activity ranged between 5.71.1 mBq kg-1 and 25.03.2 mBq kg-1. In all the samples 238Pu activity fell below the minimum detection activity, which was on the level of a single mBqkg-1, so suggesting global fallout as main source radioactive contamination in southern Poland. In case Northeastern Poland in study involved 25 people, 10 men and 15 women. Age range was between 32 to 85 years old. Minimum activity of 239+240Pu was equal to 5.41 mBq kg-1, whereas the maximum activity reached 34.35.7 mBq kg-1. In 6 samples 238Pu activity fell below the minimum detection activity, in rest activity was between 1.91.4 to 10.63.1 mBq kg-1. The measurable amounts of 238Pu suggest presence of traces of Pu of Chernobyl origin in bodies of inhabitants of Northeastern Poland.

Speaker: Mr Kamil Brudecki (The Henryk Niewodniczański Institute of Nuclear Physics, Polish Academy of Sciences)

125 Comparison of metal accumulation in tree bark and soil from urban parks in São Paulo city, Brazil

The main sources of air pollution in the São Paulo megacity are gases and particulate matter released by the ever increasing fleet of light and heavy vehicles (more than 7 million) as well as industrial process emissions. These emissions are of great concern due to their effects on human health, causing lung cancer and respiratory problems, since they contain a wide range of potentially toxic metals and organic contaminants. In the present paper, the concentration levels of the metals Ba, Co, Cr, Cu, Fe, Ni, Pb and Zn in superficial soil and tree bark samples collected in urban parks of São Paulo city were determined and compared. The analytical techniques employed were neutron activation analysis and X-ray fluorescence spectrometry. Higher concentrations of Ba, Cr, Cu, Pb and Zn were obtained both in the soil and bark trees samples in relation to reference values, in the case of soils, and to a control area, in the case of the tree barks, indicating the influence of anthropogenic sources. Statistical analysis applied to the soil and tree barks concentration data showed that the studied metals presented the same behavior in the soil as well as the tree bark samples. There was an association between the traffic-related metals Cu, Zn and Pb, suggesting that these three metals originate from vehicular emissions. The utilization of these two different environmental compartments for pollution monitoring may improve the comprehension of metal pollution in urban parks in megacities, in order to identify the emission sources and to implement pollution-control strategies

Speaker: Dr Ana Maria Figueiredo (IPEN-CNEN/SP)

Poster Poster_Ana_4.pdf

126 Correlation study of air pollution and cardio-respiratory system diseases through NAA of atmospheric pollutant biomonitor

Atmospheric pollution is today one of the many problems facing mankind. This problem affects everything from the natural environment to human health and to climate. As result authorities of all over the world have become very preoccupied with the adverse effects derived from air pollution. The objective of this study was to apply Neutron activation Analysis (NAA) to collect air pollution data in the city of São Paulo, Brazil in order to investigate pollutant effects on cardio-respiratory system. Canoparmelia texana lichenized fungii species was chosen for passive biomonitoring of atmospheric pollutants. The two population groups selected for this study were, one of children under 5 years and the other of adults over 45 years. Lichen samples collected in São Paulo city were cleaned, freeze-dried and ground for the analysis. Aliquots of samples were irradiated at the IEA-R1 nuclear research reactor for short and long periods along with synthetic element standards. The induced gamma activities of the samples and standards were measured using a gamma ray spectrometer with an HPGe detector and the concentrations of As, Ba, Br, Ca, Cd, Cl, Co, Cr, Cs, Fe, Hf, K, Mg, Mn, Na, Rb, Sb, Sc, Se,Th, V, Zn and lanthanides were determined. For quality control of the results, certified reference materials were analyzed. Mortality data for the population due to cardio-respiratory diseases were obtained from the database of the Secretariat of Health of the São Paulo Municipality for the years 2005 to 2009. Results obtained indicated that the origins of pollutants in São Paulo city are due to vehicular and industrial emissions. The statistical treatment of Pearson´s correlation applied to the results of lichen element concentrations and mortality rates indicated significant positive correlation for the elements Co, Mn and Zn for adults.

Speaker: Dr Mitiko Saiki (Instituto de Pesquisas Energéticas e Nucleares)

Paper ID_41-SAIKI.doc ID_41-SAIKI.pdf

Poster MITIKO_SICILY_2011.pdf

127 Determination of short-lived radionuclides in neutron-activated urban atmospheric Particulate Matter

Many studies have focused their attention on the determination of elements of toxicological and environmental interest in atmospheric particulate matter using analytical techniques requiring chemical treatments. The Instrumental Nuclear Activation Analysis (INAA) technique allows to achieve high sensitivity, good precision and excellent limit of detection without pre-treatment, also considering the problems related to the radioisotope characteristics (e.g., half-life time, interfering reactions, spectral interferences). In this communication elements such as Al, Br, Cl, Cu, I, Mg and V, are studied in atmospheric PM10 sampled in downtown Rome: the relative radionuclides are characterized by short half-lives (ranging from 2.31 to 37.9 min). Further, As, La, Mn and Sb were also determined for evaluating the toxicological aerosol characteristics. Samples and standards were irradiated for 20 min in the pneumatic channel of the TRIGA Mark II nuclear reactor of Casaccia ENEA, at a total neutron flux of 1.25×1013 n×cm-2×s-1; the γ-measurement times were 10 and 80 min according to the radioisotope properties. The results, elaborated considering the matrix effects and the interfering reaction contribution to the radioisotope formation (e.g., 28Al generated by (n,γ) reaction from 27Al and by (n,p) reaction from 28Si), show intersting values of As (0.3-6.1 ng m-3), Cu (22-313 ng m-3), Mn (17-125 ng m-3), V (7-63 ng m-3), higher than those determined in an area not influenced by autovehicular traffic. The other elements show a pattern similar to the very few data present in literature. It should be underlined the good correlation of Al vs Mg (0.915) and La (0.726) indicating a same sources for these three species, whereas the Br-Sb trend shows a minor correlation (0.623) meaning different contributions to their levels.

Speaker: Dr Pasquale Avino (INAIL (ex-ISPESL))

128 Determination of Sr-90 and Pb-210 in freshwater fish in Austria

A method for the determination of 90Sr and 210Pb in freshwater fish was developed. The determinations were conducted within a project on behalf of the Federal Ministry of Health. The aim of this project was to get an overview of natural radionuclides and artificial radionuclides in freshwater fish in different lakes in Austria. For sampling the Neusiedler See in Burgenland, two lakes in Styria the Grundlsee and the Toplitz See and the Zeller See in Salzburg were chosen. Chub (leuciscus cephalus), pike (esox lucius), perch (perca fluviatilis), carp (cyprinus carpio), catfish (silurus glanis), pike-perch (sander lucioperca) and burbot (lota lota) were analysed. The fish sample was ashed and dissolved in concentrated HNO3 with intermittent additions of H2O2. After ammonium oxalate precipitation the 90Sr and 210Pb precipitate was washed with water and then the oxalate was destroyed by fuming off with concentrated HNO3. 90Sr and 210Pb were separated with strontium specific extraction columns from Triskem. 90Sr was stripped from the column with 0.05 M HNO3 and 210Pb with 0.1 M ammonium oxalat solution. Measurements were conducted with a Quantulus 1220. For the determination of the chemical recovery first the initial strontium and lead concentration in the sample was measured and then a Sr(NO3)2 and Pb(NO3)2 carrier solution was added. The strontium and lead concentrations were measured with ICP-MS. In this paper the method for the determination of 90Sr and 210Pb is described and the results are discussed.

Speaker: Claudia Landstetter (Austrian Agency for Health and Food Safety)

Paper ID_43_Manuskript.doc ID_43_Manuskript.pdf

Poster ID43_-_AGES_PPT_Fisch.pdf

129 Development and characterisation of a new miniaturised detector for in vivo dosimetry in HDR brachytherapy.

Due to the recent development of new conformal radiotherapy techniques, it’s important to generate an improvement of dosimetric instruments especially in brachytherapy, in order to obtain a remarkable improvement of the measurement accuracy and precision of the absorbed dose both by healthy and pathologic tissues. The HDR brachytherapy requires the use of an interstitial implant or an intracavitary applicator where an Ir-192 source runs with its highest activity (10Ci) and gradient. The interest in in-vivo measurement of the dose delivered to the target or to the neighbouring healthy organs is getting higher, due to the strong complexity of the treatment. For this reason a real time miniaturized system for in-vivo dosimetry based on a Ce3+-doped SiO2 optical fibre is now under study. A careful analysis was made in order to define one of the most important aspects of the measurement process: the detector sensibility connected to the source distance, to the dose rate and to the radiation incidence angle. The results of that investigation were very encouraging as they have proved a very good response linearity of the detector with the dose such as the independence of the response from energy and dose rate. Moreover it was tested that the response of the detector depends on the irradiation temperature with consequent determination of the correction factor. The results indicate that the use of this new system is very promising both for quality control measurements and in-vivo dosimetry, especially for gynaecological and prostatic treatments.

Speaker: Prof. Grazia Gambarini (Department of Physics, Università degli Studi, Milan, Italy and INFN Istituto Nazionale di Fisica Nucleare, Milan, Italy)

Poster poster_sicily.pdf

130 Distribution of heavy metals in fish tissues of the Tepuxtepec Dam, Mexico

The Lerma River is born near the Toluca city. This city has an industrial, commercial and agricultural activity, the river then continues their flow to the Tepuxtepec dam which is used as a water reservoir and fish production for the local population. The concentration of heavy metals (Cr, Ni, Cu, Zn, Cd, Hg and Pb) in gills, liver, kidney and muscle of herbivorous carp (Ctenopharygodon idella) from Tepuxtepec Dam, Mexico was evaluated. The samples were collected from six regions in the dam and analyzed in triplicate by X Ray Fluorescence technique. A TXRF spectrometer “TX-2000 Ital Structures” with a Si(Li) detector and a resolution of 140 eV (FWHM) at Mn Kα. A Mo tube (40 kV, 30 mA) with 17.4 KeV excitation energy was used. The mean concentration in tissues decrease in the sequence: Kidney ≈ Gills > Liver > Muscle; the range of concentration for Zn was 26.68-816.67 mg/Kg followed by Cu: 1.18-35.81 mg/Kg, Cr: 1.20-5.80 mg/Kg, Cd: 0.30-7.00 mg/Kg, Ni: 0.40-3.70 mg/Kg, Pb: <0.02-1.92 mg/Kg and Hg: <0.03-1.14 mg/Kg. Chromium and mercury concentrations slightly exceed the limits for fish proposed by FAO/WHO and Mexican legislation for human consumption in the edible parts of fish from each one of the regions of the Tepuxtepec dam. The results show that metal accumulation in herbivorous carp tissues was higher in regions 3, 4 than the others, which could be due to the influence of Lerma River, one of the most polluted rivers of Mexico.

Speakers: Dr Graciela Zarazua (Instituto Nacional de Investigaciones Nucleares), Prof. Trinidad Martinez (UNAM. Facultad de Ciencias)

131 EBT2 radiochromic films for absolute dose measurements in radiotherapy: prototype of an innovative system for their analysis

One of the most important progress reached in radiotherapy in the last decade is intensity modulated radiation therapy (IMRT). This modern radiotherapy permits to achieve a conformed high dose distribution around the target volume, sparing at the same time the surrounding critical organs and healthy tissues. Since the radiation fields are very complex and the absorbed doses during IMRT treatments are very high, it’s important to verify the effective dose distribution. Usually dose distribution verification is obtained by two dimensional detectors, such as diode or ion chamber arrays, or by film dosimetry. Film dosimetry is more time consuming if compared to detector arrays, but has the important advantage of gathering higher spatial resolution. The new GAFCHROMIC® EBT2 is the most modern film dosimeter. Previous GAFCHROMIC® film dosimeters, EBT, were modified to decrease their response dependence on energy and dose rate. GAFCHROMIC® EBT2 has a good dose and spatial resolution; therefore it’s convenient to design a new analysis system more sensitive and precise than commercial scanners. The proposed system is composed by a planar uniform white light source and a CCD camera with an optical filter around 630nm. The system has been set up and optimized to achieve GAFCHROMIC® EBT2 analysis. A measure procedure was established to investigate EBT2 dose response over the adopted range of energies as well as to evaluate EBT2 sensitivity variation as a function of time after irradiation. Finally, absolute dosimetry of complex IMRT radiation fields was achieved with EBT2 films. Obtained results have been compared to treatment planning system calculations and the goodness of the proposed system has in such way confirmed.

Speaker: Dr Nicole Mantaut (Università degli studi di Milano)

132 Evaluation of Y-90 labeled PANAM dendrimers of the 1st and 4th generations

Radiolabeled monoclonal antibodies and their fragments represent promising agents for radioimmunotherapy of cancers. For labeling with radiometals, macrocyclic chelating agents with high complex stability are usually attached to the biomacromolecule. To achieve specific activity of the antibody sufficient for a cancer treatment, large numbers of chelating groups have to be conjugated to a single macromolecule that usually results in a drop of its immunoreactivity. The problem could be overcome by an employment of biocompatible dendrimer-based agents. Dendrimers are hyperbranched artificial macromolecules with tree-like structure enabling multifunctional modification of their surface. The purpose of this study was to optimize the procedure for radiolabeling with Y-90 of PANAM dendrimers of the first (G1) and fourth generation (G4) conjugated with a DOTA derivative DO3A-py/NO-C/ (10-/4-carboxy-1-oxidopyridin-2-yl/methyl-1,4,7,10-tetraazacyclododecane-1,4,7-triacetic acid) and to analyze stability of the labeled products. 8 and 57 chelators were conjugated to a single G1 and G4 molecule, respectively. For the analysis, thin-layer chromatography and size exclusion chromatography were used. Results showed that 90Y-labeled dendrimers G1 and G4 conjugated with DO3A-py/NO-C/ can be prepared with a high specific activity and radiochemical purity at 37°C. Radiolabeled species were stable for at least 24 hrs both in saline and in plasma. Our results indicate that an employment of dendrimer-radiometal chelate conjugates represents a prospective way for radiolabeling of antibodies and their fragments to obtain markedly high specific activity and minimal loss of their immunoreactivity. The work originated within Action COST BM 0607 and was supported by Czech Ministry of Education Grant No. OC08006 and by the Grant Agency of Czech Republic – grant No. P304/10/1738.

Speaker: Prof. Milan Laznicek (Charles University, Faculty of Pharmacy, Hradec Kralove, Czech Republic)

133 Experimental cross sections for Be-7 production in Al, Si, Mg and C by deuteron irradiations up to 50 MeV

With the advent of high power, high energy deuteron accelerators used for instance for the neutron source of the IFMIF facility detailed analysis of activation products in structural materials receives an increased attention (Fusion Evaluated Nuclear Data Library FENDL 3.0 ; http://www-nds.iaea.org/fendl3/). A particular case is the formation of 7Be in light, so called low activation elements. The presence of this radionuclide with T 1/2 = 53.12 d, emitting a unique -line of 477 keV (10.5 % abundance), can represent a heavy radiation burden for maintenance personnel. In order to make a realistic estimation of deuteron produced activities in collimators, beam stops and mechanical setups made from C, Si and Al different stacks containing foils of these materials were irradiated with 50 MeV beams. The 7Be content, measured with HPGe spectroscopy, allows to determine the excitation function of the X(d, 7Be)Y reactions. Also Mg samples were studied in the same way. A comparison with the scarce literature values is made. Thick target yields were derived from fits to our cross sections and integrated personnel dose was calculated for different irradiation cycles and exposure scenarios. Apart form the radiation protection issue knowledge of the excitation function of this cluster emission is of interest for testing the prediction capabilities of different model codes and to compute depth-activity curves for application in Thin Layer Activation procedures.

Speaker: alex hermanne (Vrije Universiteit Brussel)

134 Fabrication and thermo-mechanical characterization of HEMA grafted UV photo-cured biodegradable chitosan film

Life is polymeric in its essence: the most important components of living cell (proteins, carbohydrates and nucleic acids) are all polymers. Nature uses polymers both for construction and as part of the complicated cell machinery. Development of polymer is a continuous process for achieving polymer in a specific application under certain environmental condition. The bombardment of the invention of different polymer field is increasing day by day. The natural polymer is biodegradable, easily decomposable and environmentally friendly. Natural polymer, chitosan was extracted from dried prawn shell waste through the preparation of chitin and was characterized by FTIR. Thin film of chitosan was prepared by casting from its 2% chitosan in 2% acetic acid solution. Mechanical properties like tensile strength (TS), elongation at break (Eb) of chitosan film were studied. Eight formulations (M1: 5% HEMA to M8: 40% HEMA) were developed with 2-hydroxyethyl methacrylate (HEMA) monomer in methanol along with photoinitator Darocur-4043 (2%). The film was soaked in those formulations in dissimilar soaking times and irradiated under UV radiation at different radiation intensities for the improvement of physico-mechanical properties of the films. The cured films were then subjected to various characterization tests like Fourier Transformed Infrared Spectroscopy, Polymer Loading (PL), Tensile Strength (TS), Elongation at Break (Eb), Differential Thermal Analysis (DTA), Thermo gravimetric Analysis (TGA) and Water Uptake Tests. The formulation (M6) containing 30% HEMA showed the best performance at 20th UV pass for 1 min soaking time. The highest TS, Eb and PL were found to be 31MPa, 71.25% and 26.38%, respectively, for the same formulation at 20th UV pass for 1 min soaking time. The DTA/TG study showed that the film with M6 formulation at 20th UV pass for 1 min soaking time was more thermally stable than non-radiated chitosan film and the other monomer formulations. The FTIR analysis revealed the crosslinking between HEMA and chitosan. This study creates a new field of research on chitosan using acrylic monomers and UV radiation to improve the inherent chitosan films properties for biomedical application.

Speaker: Mr Kamol Dey (Department of Applied Chemistry & Chemical Engineering, University of Dhaka, Bangladesh)

135 Gamma-ray spectroscopic characterization of radioactive preparation for production process validation in a PET cyclotron facility

Introduction The Pharmaceutical Industry in European Community applies very strict rules for quality assurance in production and control of pharmaceuticals. A manufacturer’s authorization guarantees that all authorized pharmaceuticals satisfy the Good Manufacturing Practice (GMP) requirements for medicinal products. Many national Governments have created their own GMP guidelines. In Italy, the supplement of Gazzetta Ufficiale of Italian Republic n° 274 (23 November 2010) states the guidelines to define and to control manufacturing processes, and for inspections in pharmaceutical laboratories. One of the requirements is related to validation: a new process or after significant changes to the facilities, the equipments or the process, which may affect the quality of the product, should be validated. This validation is requested to verify the accuracy of parameters included in the process and the reproducibility. GMP guidelines fixes to 0.1% for 18F and 1% for 11C and 13N the limits of the total radioactivity due to radionuclide impurities present in the pharmaceutical preparation at the administration time. In this study gamma-ray spectroscopic characterization of radioactive preparation from proton bombardment for production process validation of 11C, 13N and 18F are presented. Materials and methods The PET centre at San Raffaele Scientific Institute is equipped with two cyclotrons, IBA Cyclone (18/9 MeV) and CTI Eclipse (11 MeV). 11C is produced with both cyclotrons by 14N(p,n)11C nuclear reaction with Al target and Havar foils (CTI) or Al foils (IBA), respectively. With CTI 12.4±0.2 GBq are produced with a 60 min irradiation at a beam current of 25 microAmpere, while with IBA 59.7±5.3 GBq are produced with a 60 min irradiation at a beam current of 35 microAmpere. 13N is produced with CTI by 16O(p,alpha)13N nuclear reaction with Al target and Ti foils. Produced 0.23±0.01 GBq/ml, with a 20 min irradiation at a beam current of 40 microAmpere. 18F is produced with both cyclotrons by 18O(p,n)18F nuclear reaction: CTI uses Ag/Nb target (dual bombardment) and Havar foils, while IBA uses Nb target and Havar foils, respectively. With CTI 2.1±0.2 GBq/ml are produced with a 60 min irradiation at a beam current of 20 microAmpere, while with IBA 0.7±0.1 GBq/ml are produced with a 10/12 min irradiation at a beam current of 32 microAmpere. Spectroscopic measurements were performed using an High-Purity Germanium detector with 18% relative efficiency and 0.14% energy resolution at 1332 keV. Detector calibrations were performed with 152Eu and 133Ba certified sources. For the detection and quantification of impurities, the preparations were examined, after an adequate time to allow the decay of nuclide to a level that permits the detection of impurities, for at least 24 hours. The measured activity values were normalized at the end of bombardment and to the preparation volume. Results Analysis of produced radioactive preparations showed the presence of impurities: 44Sc, 44mSc, 46Sc, 47Sc, 48V, 52Mn, 56Co for a 13N sample, 52Mn, 54Mn, 56Co, 57Co, 58Co, 67Ga, 109Cd for a 18F-CTI sample and 51Cr, 52Mn, 55Co, 56Co, 57Co, 57Ni, 58Co, 67Ga for a 18F-IBA. No nuclide was detected on 11C sample of both cyclotrons. The 13N sample showed also the presence of 18F, identified with its lifetime. Measured impurities activities ranged from 120 Bq to 700 Bq, resulting in 2.7±0.1•10-6 % for 13N, 6.9±1.5•10-7 % for 18F-CTI and 4.0±1.4•10-6 % for 18F-IBA. The type of radionuclides found in this study are inherent with the targets and foils employed for proton irradiation. In particular Sc is likely obtained from the nuclear reaction Ti(p,x)Sc, 48V from 48Ti(p,n)48V, all Co isotopes from natFe(p,x)Co or natNi(p,x)Co, Mn isotopes from 54Fe(p,x)Mn, 51Cr from 54Fe(n,alpha)51Cr, 57Ni from 58Ni(p,d)57Ni, 67Ga from 67Zn(p,n)67Ga and 109Cd from 109Ag(p,n)109Cd. Conclusion Measured activities of impurities are much less than the fixed limit, therefore the production processes of 11C, 13N and 18F can be considered validated concerning the radionuclide purity. We conclude that our production processes have a high degree of confidence and can permit to detect and correct deviations which could cause problems during nuclide production.

Speaker: Dr Ignazio Vilardi (Nuclear Medicine Department, Multimedica Scientific Institute, Sesto San Giovanni (MI), Italy)

136 Hyaluronic acid labeled with radioiodine: Optimization of labeling procedure and preclinical evaluation

Hyaluronic acid (HA) is a high molecular weight glycosaminoglycan composed of repetitive disaccharide units. HA participates in various physiological and pathological processes in the body and is typically used as a medical device, dietary supplements etc. Ubiquitous in all tissues and fluids, the fate of exogenously administered HA in the body cannot be directly determined by any classical analytical method. Labeling of HA with radiotracer is one of the few ways to determine the fate of HA in the organisms. The aim of this work was to label HA by radioiodination via prosthetic group of reactive aromatic amino acid residues thyrosine and tyramine and to determine biodistribution profiles of 125I-labeled HA in rats. For labeling of adducts of HA with tyrosine and tyramine, oxidative iodinatation was employed. The higher radiochemical yield for HA-tyramine adduct was reached in comparison with HA-tyramine. Reaction products were purified by molecular size exclusion chromatography and administered intravenously to male Wistar rats. Biodistribution profile of both agents was characterized by a rapid uptake from the bloodstream by the liver mediated by CD44 receptors and by relatively long liver radioactivity wash-out time. In the liver, both HA adducts under study were partly degraded and the fragments redistributed in the body. The main elimination pathway was radioactivity excretion to the urine. The results might be usable for a better understanding of biological behavior of HA in the body. This study was supported by the the grant of Ministry of the Czech Republic No.OC08006 as well as by CPN s.r.o, Dolni Dobrouc.

Speaker: Dr Alice Laznickova (Charles University, Faculty of Pharmacy, Hradec Kralove, Czech Republic)

137 In-vivo dosimetry in HDR brachyterapy with Fricke-gel catheters: preliminary results

In-vivo dose measurements during complex conformal radiotherapy treatments are very important, in order to check the dose delivered to the patient and compare this dose with the prescribed one, improving in such a way the treatment quality. A method has been studied and developed aimed to perform in vivo dosimetry during brachytherapy treatments. The method is based on a radiochromic Fricke-gel injected in plastic catheters with length of 14 cm and external diameter of 0.3 cm. The gel is infused with a modified Fricke solution, having the following composition: ferrous sulphate solution [1mM Fe(NH4)2(SO4)2 · 6H2O], sulphuric acid [25mM H2SO4] and Xylenol-Orange [0.165mM C31H27N2Na5O13S]. The gelling agent was Agarose, in the amount of 3% of the final weight. Ionizing radiation produces a conversion of ferrous ions to ferric ions whose yield is proportional to the absorbed dose. The absorption spectrum of the chemical compound XO-Fe3+ has a peak around 585 nm, whereas the absorption spectrum of the non-bounded XO molecule has a peak around 430 nm. The dosimeter analysis is executed evaluating the variation in optical density, in the region of wavelengths around 585 nm, of the optical transmittance images detected by a CCD camera. Proper software was developed, to achieve light absorbance through dosimeters having cylindrical shape. After having outlined a suitable analysis protocol and developed the due software, the dose-response curve was studied. Finally, in-phantom measurements have been carried out, with a Microselectron (Nucletron, Veenendaal, The Netherlands) high dose-rate remote afterloading device. The resulting dose profiles were compared with the dose values calculated by the treatment planning system (TPS) along all the dosimeter position and the reliability of the proposed method was confirmed.

Speaker: Prof. Grazia Gambarini (Università degli Studi di Milano and INFN, Milan, Italy)

138 In-vivo dosimetry in prostate HDR brachytherapy with thermoluminescence detectors (TLDs)

During complex conformal radiotherapy treatments it is very important, also if not mandatory, perform in-vivo dose measurements. In fact, in-vivo dosimetry allows monitoring the dose delivered to the patient and to compare this dose with the prescribed one, improving in such a way the quality assurance. Currently, the most utilised methods for the in-vivo dosimetry are based on thermoluminescent detectors (TLDs) and silicon diodes. TLDs are sometimes preferred, for small size (in this case 3x3x0.9 mm3), the lower dependence of the response on photon energy, the dose rate and the direction of incidence. In external beam radiotherapy, the dosimeters are placed on the patient’s skin, in suitable positions in order to perform measurements at entrance and exit points. For brachytherapy, where treatments are carried out introducing the source within the patient's body, in-vivo measurements inside the patient are required. A method for performing in-vivo dosimetry inside the patient body during brachytherapy treatments using LiF:Mg,Ti (TLD-100) has been studied and set up. A TLD calibration protocol has been defined, aimed at achieving absorbed dose values with the due precision. Some calibrated TLDs were used to perform control measurements during the brachytherapy treatments of the prostate in a few patients with the 192Ir source of a Microselectron-HDR high dose rate remote afterloading device. Five TLDs were fixed to the echographic probe that remains inside the patient during the treatment. The results have been compared with those calculated by the treatment plane software (TPS) and the consistency of the technique has been verified.

Speaker: Dr Simone Alessandro Grisotto (Physics Department of the Università degli Studi, Milan, Italy)

Poster 144_poster_grisotto.pdf

139 Instrumental Neutron Activation Analysis applied to multielement determination in lettuce grown in phosphate treated contaminated soil

In recent decades, anthropogenic activities, particularly those associated with industrial processes and mining, have been the major source of inorganic element enrichment in soils. Unlike organic contaminants, most inorganic elements do not undergo microbial or chemical degradation therefore their total concentrations remain in soils for a long time after their apparence. In this case, due to the possibility these elements present at toxic levels to plants which can reach the food chain, the interest in developing of technologies for remediating contaminated sites has increased. The addition of substances capable of immobilizing toxic elements in the soil is a procedure that has been used for remediating contaminated sites. The purpose of this study was to evaluate the efficiency of super phosphate in the treatment of a soil contaminated with elements that can be potentially toxic. Different doses of super phosphate (250, 500, 1000, 2000 and 4000 mg kg-1 of P) were added to a number of lettuce plant pots contain contaminated soil. The element concentrations absorbed in the leaves from lettuce treated with phosphate were compared with those absorbed in the leaves of a control plant. Instrumental neutron activation analysis (INAA) followed by gamma-ray spectrometry was the analytical method used to determine element contents in the lettuce leaves. The use of 250 mg kg-1(P) proved to be the most effective treatment to reduce the concentrations of Br, Ca, Cd, Cl, Co, Fe, K, Mg, Mn, Sb and Zn in lettuce leaves.

Speaker: Dr Mitiko Saiki (IPEN/CNEN-SP)

Paper ID_58.doc ID_58.pdf

Poster Poster-Sicilia.pdf

140 Kinetic and thermodynamic analysis for the absorption of U(VI) on the crosslinked polyester resin with acrylic acid from aqueous solutions

Uranium and its compounds are highly toxic which causes progressive or irreversible renal injury and in acute cases may lead kidney failure and dead (1-3). For this reason, many removal processes have been used for adsorption of radioactive metal ions such as uranium(VI), strontium(II) and cesium(I) ions from industrial waste waters and waste solutions (4-6). Organic and inorganic adsorbents have been used for removal processes of radioactive metal ions from wastes. In recent years, polymeric adsorbents have indicated an increase for the treatment of aqueous nuclear waste solutions due to controlling adsorption capacity and supplying selectivity in adsorption processes (7-9). For this purpose, 80 g of unsaturated polyester resin (Polipol 353, Poliya) were mixed with 20 g of acrylic acid. This mixture was copolymerized using cobalt octoate (0.5 mL of 1%Co in toluene)-methyl ethyl ketone peroxide((1 mL of Butanox M60) initiator system at room temperature. In this study, the effects of the contact time, temperature and U(VI) concentration for the adsorption of U(VI) on the crosslinked polyester resin bearing acrylic acid functional groups have been investigated. The adsorption data have been well represented by the Freundlich, Langmuir and Dubinin-Radushkevich (D-R) isotherms. The adsorption capacity of the crosslinked copolymer and free energy change are calculated by using D-R isotherms. Thermodynamic parameters (∆H0, ∆S0 and ∆G0) have been determined for the adsorption of U(VI) ions on the crosslinked copolymer bearing acrylic acid functional groups from aqueous solutions. Experimental adsorption data have been analyzed using sorption kinetic models such as the Elovich, fractional power, pseudo-first order and pseudo-second order kinetic models. It has been observed that pseudo-second order kinetic model provided a high degree of correlation with experimental data for the adsorption of U(VI) ions on the crosslinked copolymer bearing acrylic acid functional groups from aqueous solutions References 1. Mellah A. Chegrouche S. and Barkat M., J. Colloid and Interface Sci. 296 434 (2006). 2. Rao T.P., Metilda P. and Gladis J.M., Talanta 68 1047 (2006). 3. Qadeer R. and Hanif J., Radiochim. Acta 65 259 (1994). 4. Özeroğlu C.ve Keçeli G., J. Radioanal. Nucl. Chem. 268(2) 211 (2006) 5. Singh B.N. and Maiti, B., Talanta, 69 393 (2006) 6. Özeroğlu C. ve Keçeli G., Radiochim. Acta 95 1 (2007). 7. Maheswari M. A. and Subramanian M.S. React. Funct. Polym. 62(1) 105 (2005) 8. Büyüktiryaki S., Say R., Ersöz A., Birlik E. and Denizli A., Talanta 67 640 (2005). 9. Özeroglu C., Keçeli G., Radiochim. Acta 97 709 (2009).

Speaker: Dr Cemal OZEROGLU (Istanbul University Faculty of Engineering Department of Chemistry 34320 Avcilar-Istanbul/TURKEY)

141 Metal and trace element assessment of Tietê river sediments, São Paulo, Brazil

The Tietê River is one of Brazil’s most important rivers and crosses the State of São Paulo (SP) from east-to-west flowing into another important river, the Paraná River. The objective of this study was to quantify the amount of trace elements and some metals present in sediments collected from the Tietê River, at 5 different sampling points (P0-P4), in 3 campaigns (2008/2009), from the headwaters to Suzano County upstream from São Paulo city. Instrumental Neutron Activation Analysis was applied for measuring total concentration of some metals and trace elements. The USEPA 3051 digestion procedure was used for sediment digestion and determination of Cd, Cu, Cr, Ni, Pb and Zn by inductively coupled plasma optical emission spectrometry (ICP OES) and Hg by cold vapor atomic absorption spectrometry (CV AAS) were carried out. The metal concentrations obtained by acid digestion were compared to concentrations established by CONAMA 344 (Brazilian legislation) for evaluating the potential effects on aquatic organisms. The sampling sites P3 and P4, near industrialized areas, showed the highest concentrations for potentially bioavailable metals, mainly Zn and Hg. Zn concentrations at sampling P3 and P4 were 390 and 590 mg kg-1 respectively, well above CONAMA level 2 ( 315 mg kg-1). Mercury was found in the range of 0.411- 0.448 mg kg-1 close to CONAMA level 2 (0.486 mg kg-1). Cd, Cu, Cr and Pb were also detected above CONAMA level 2 concentrations in at least one of these two sampling points. The results obtained by INAA were compared to earth crust values. The enrichment factor in relation to earth crust values using Sc as a normalizer element was also calculated. A strong enrichment was found for the elements As, Br, Sb, Th, U and Zn. These results evidenced contamination by industrial effluents and sewage even relatively close to the Tietê River headwaters. The worst biological effects (acute toxicity) were also observed at P3 and P4.

Speaker: Deborah FAVARO (Instituto de Pesquisas Energeticas e Nucleares)

Paper ID_52_FAVARO_INCC_Paper_JRNC.doc ID_52_FAVARO_INCC_Paper_JRNC.pdf

Poster Favaro_3rd_INCC_190811.pdf

142 Microspheres with an ultra high holmium content for brachytherapy of malignancies

The overall objective of this work is to develop biodegradable microspheres intended for internal radiation therapy which provides an improved treatment for hepatic carcinomas [1]. The most studied brachytherapy systems employing microspheres made of holmium-biopolymer system, is composed by poly(L-lactic acid) (PLLA) and holmium acetylacetonate (HoAcAc) [2]. The importance of the holmium high content in the microspheres can be interpreted as follows: a) From a therapeutic standpoint, for effective use of microspheres loaded with the complex, it requires a high content of holmium to yield enough amounts of radioactivity with a relatively low amount of microspheres; b) From the viewpoint of the microspheres irradiation, namely, small quantities of holmium-165 would require longer irradiation times to the polymers, which would be subjected to undesirable radiation doses of the reactor core [2, 3]. The usual amounts of holmium that are incorporated in the microspheres composed by poly(L-lactic acid) and HoAcAc are 17.0 ± 0.5% (w/w) of holmium, which corresponds to a loading of about 50% of HoAcAc [3]. Different approaches have been investigated to increase that value. One updated approach towards this direction, is the production of microspheres with ultrahigh holmium as matrix using HoAcAc crystals as the sole starting material without the use of biopolymer [4,5]. Likewise, in the process searching for the increase of the holmium content in the microspheres, it has been demonstrated that by changing the HoAcAc crystal structure by its recrystallization from crystal phase to the amorphous there is lost of acetylacetonate and water molecules causing the increasing of the homium content. Microspheres were prepared by solvent evaporation, using holmium acetylacetonate (HoAcAc) crystals as the sole ingredient (A). Microspheres were characterized by using light and scanning electron microscopy (B), infrared and Raman spectroscopy, differential scanning calorimetry, X-rays difration (C) and confocal laser scanning microscopy(CLSM). References: [1] Renata F. Costa, Mariangela B. M. Azevedo, Nanci Nascimento, Frank F. Sene, José R. Martinelli, João A. Osso International Nuclear Atlantic Conference - INAC 2009, ABEN ISBN: 978-85-99141-03-8; [2] Nijsen J. F. W. et al. Eur. J. Nucl. Med., 26, 699-704, 1999; [3] Zielhuis S. W. et al. Intern. J. Pharma., 311, 69–74, 2006; [4] Bult, W. et. al. Pharma. Res. 27, 2205-2212, 2010; [5] Pharm. Res. 26, 1371-1378, 2009.

Speaker: Dr MARIANGELA BURGOS M. de AZEVEDO (IPEN/CNEN)

143 Nanozeolites as carriers for radium radionuclides.

Objectives: The aim of the work was to study the possibility of using nanozeolites as carriers for very perspective therapeutic radionuclides -emiters 223,224,225Ra. These metals do not form stable complexes so they can hardly be bound to biomolecules via chemical bonds. Zeolites are crystalline aluminosilicates composed of tetrahedral elements that build open framework structures - a system of channels and cages of molecular dimensions [1]. Moreover, these molecular sieves are good ion exchangers with high affinity to mono and divalent cations, therefore radium radionuclides can be easy encapsulated inside the zeolite structure. Methods: Nanozeolites were synthesized by hydrothermal method [2]. The synthesis was conducted in a temperature controlling magnetic stirrer. Chemical reagents included sodium hydroxide (Chempur), aluminum hydroxide (Aldrich), colloidal silica 45 wt. % suspension in water (Ludox CL-X, Aldrich), fumed silica (Aldrich), distilled water. Aluminate and silicate solutions were mixing together in the molar ratio 5.5 Na2O : 1.0 Al2O3 : 4.0 SiO2 : 190 H2O to obtain faujasite (FAU) or NaX type of zeolite. The influence of silicate source, aging time of precursor sols, rotation rate and temperature on the size of final nanozeolite have been studied.In the preliminary experiments the obtained samples were examined for adsorption of 133Ba which was used as the model for 223,224,225Ra. Result: The studied nanozeolites exhibited high affinity for both 133Ba. The distribution coefficient value for 133Ba exceeds 104 cm3•g-1. The stability of radiolabelled nanozeolites was studied in various solutions containing: physiological salt, competitive cations (K+, Ca2+), complexing agent (EDTA) or buffer (PBS). The leakage of 133Ba from the nanozeolites was below 0.2%. In the next stage, 224Ra (milked from 228Th/224Ra generator) was absorbed in the nanozeolites. No leakage of activity to the solution after shaking NaX-224Ra with 0.9% NaCl, 0.02 M PBS, 10-3 M KCl, 10-3 M CuSO4 was observed. The only exception was for EDTA (the leakage was above 50%). Thus, in the next step, the same sample was examined in human serum. About 15% of -radioactivity was found in the solution, which has been attributed to 212Pb - the decay product of 224Ra. Conclusions: Nanosized zeolites were successfully prepared via hydrothermal synthesis. The nanozeolite NaX exhibits high affinity for 224Ra. In the future experiments nanozeolites of other types, with smaller cages and channels, will be synthesized. The studies on their stability in vitro will be continued. References 1. Grieken R. V., Sotelo J. L., Menendez J. M., Melero J. A., Microporus and Mesoporous Materials, 39, 135-147, (2000); 2. Zhan B.-Z., White M. A., Robertson K. N., Cameron T. S., Gharghouri M., Chem. Mater., 14, 3636 – 3642, (2002).

Speaker: Prof. Aleksander Bilewicz (Institute of Nuclear Chemistry and Technology)

144 Native and transplanted lichen and bark as air pollution biomonitors at three different meteorological conditions

At three sites of Portugal – Viana do Castelo, Sacavém, Sines – bark from Olea europea and the lichen Parmelia caperata, collected in clean areas, were exposed. The situation of the sites allows different meteorological conditions, from rainy to dry and cooler to warmer. Three different procedures for the lichen exposure were adopted: rectangular flat pieces, the lichen in its original form and biomass (previously ground lichen). Samples were exposed for 9 months and removed after 3, 6 and 9 months (continuous mode) and exposed for 3 months, in a winter campaign, a spring campaign and a summer campaign (discontinuous mode). Conductivity was measured before and after exposure whenever possible. Ten samples of each biomonitor were kept for analysis prior to exposure. All samples were analyzed by Instrumental Neutron Activation analysis (INAA), at the Portuguese Nuclear Reactor, and the chemical elements were determined. Total deposition was collected simultaneously to the exposures and analyzed by inductively coupled plasma mass spectrometry (ICP-MS). Meteorological data were taken from the Portuguese Meteorology Institute and processed together with the chemical element concentrations. Results are discussed on basis of 1) influence of humidity/precipitation and temperature on bark and lichen transplant elemental accumulation, and 2) of different procedure of lichen exposure (biomass, usual one and flat - well-determined exposure area - pieces).

Speaker: Dr Maria do Carmo Freitas (Instituto Tecnológico e Nuclear, URSN)

Paper INCC_ID19_Canha.doc INCC_ID19_Canha.pdf

Slides INCC_poster.pdf INCC_poster.pptx

145 Natural radionuclides content and radon exhalation rate from brazilian phosphogypsum piles

Phosphogypsum is a waste of the wet-acid process for producing phosphoric acid from phosphate rock. For every ton of phosphoric acid obtained, from the reaction of phosphate rock with sulfuric acid, about four tons of phosphogypsum are produced. Large quantities of phosphogypsum have been produced worldwide. In 2006, annual production was estimated to be about 170 million tons. Brazilian annual production of phosphogypsum reaches 5.5 million tons. In Brazil, the major phosphgypsyum producers are Ultrafertil, located in Cubatão, State of São Paulo and Fosfertil, in Uberaba, State of Minas Gerais. Brazil, such as other countries that produce phosphate fertilizer, tries to find solutions for the safe applications of phosphogypsum, in order to minimize the impact caused by its disposal. Most of worldwide phosphogypsum is stock piled, posing environmental concerns. The monitoring of air and groundwater pollution, radon exhalation rate and direct exposure to gamma radiation for workers should be considered. The aim of this study is to evaluate the natural radionuclides content and the radon exhalation rate from phosphogypsum piles from Ultrafertil and Fosfertil fertilizer industries. Samples of this material were analyzed by high resolution gamma spectrometry for their 226Ra, 228Ra, 210Pb and 40K activity concentration. Radon exhalation rate had been measured by the charcoal canister method. A theoretical model for radon exhalation calculation, suggest by UNSCEAR, was applied in order to confirm the experimental results. The activity concentrations results are in agreement with literature values. The average radon exhalation rates and standard deviations from Ultrafertil and Fosfertil phosphogysum piles were 0.16 ± 0.07 Bq m-2 s-1 and 0.08 ± 0.02 Bq m-2 s-1, respectively.

Speaker: Dr Marcia Pires de Campos (IPEN)

Paper ID_78_INCC_full_paper_NISTI_CAMPOS_MAZZILLI.doc ID_78_INCC_full_paper_NISTI_CAMPOS_MAZZILLI.pdf

Poster Poster_INCC_MPCampos.pdf

146 New method for Sc-47 production in nuclear reactor Maria at Świerk

Problems Radionuclides with medium energy beta emission and a several day half-life are attractive candidates for radioimmunotherapy. Among the most promising in this category is 47Sc. The methods of production high activities of carrier free 47Sc was already described. Enriched 47TiO2 targets were irradiated with high energy neutrons (En>1 MeV) to produce 47Sc via the 47Ti(n,p)47Sc reaction. Authors also developed a new separation scheme based on dissolution of TiO2 target in hot concentrated H2SO4 and slow evaporation of the solution. To avoid slow dissolution and complicated separation process we propose new method based on irradiation Li247TiF6 salt and easy dissolution of irradiated target in diluted HF solution. Materials and Methods Sample of 10 mg of Li247TiF6 was irradiated for 20 h in fast neutron flux about 1014 n cm-2 s-1. The irradiated target was dissolved in 1 M HF solution. The 47Sc was separated from the target using anion exchange resin Dowex-1 with 0.4 M HF + 0.1 HNO3 solution as eluent. The eluted 47Sc fraction was 2 times evaporated with concentrated HCl and dissolved in 0.1 M HCl. The 47Sc was adsorbed on cation exchange resin and eluted with 0.5 M molar of amonium acetate. Results and conclusions Using presented procedure we obtained carrier free 30 MBq activity sample of 47Sc. The obtained samples were used for labeling DOTATATE bioconjugate with more than 90% efficiency.

Speaker: Ms Barbara Bartos (Institute of Nuclear Chemistry and Technology)

147 Radioionidation of tyrosine by the use of exchange reaction

Tyrosine is one of the 20 standard amino acids commonly takes place in the structures of animal proteins and it is required for normal functioning in humans and found in most proteins, for example in insulin. It is converted from the essential amino acid phenylalanin in the human metabolism and is a precursor of adrenaline, noradrenaline, dopamine, thyroid hormones, melanin, etc. In humans, the L-isomer of tyrosine which is the only form, that is involved in protein syntheses. However, tyrosine is considered to be a non-essential amino acid since it does not have to be taken in with the diet, but can be synthesized by the human body from chemical reactions of phenylalanine. Tyrosine is converted into dopamine and norepinephrine. Phenylalanine and tyrosine are sometimes prescribed as antidepressants, usually in combination with other herbal nutrients. In last decade, radiolabeled L-tyrosine with 123I, 125I, 18F, 11C has been subjected in interesting researches in nuclear medical applications. For example, 11C labeled L-tyrosine was used for PET visualization and quantification of protein synthesis rate and 18F radiofluorinated o-(2-18F-fluoroethyl)-L-tyrosine has showed a clinical potential in brain tumor diagnosis, 123I-L-tyrosine showed a long tumor retention in RIM rhabdomyosarcoma tumor-bearing Wag / Rij rats, 6-125I-L-tyrosine has been incorporated into the literature to be a new radiopharmaceutical which is useful in assessing cerebral amino acid transport mechanism and quantifying metabolically active DOPA decarboxylase. In this context, the radioiodination processes have become important tools for preparation of radioiodinated L-tyrosine with different iodine radioisotopes and in this study, the radioiodination of tyrosine using an isotopic exchange technique between 131I ion and 127I atom of 2-iodo-L-tyrosine has been investigated as a new radioiodination procedure of L-tyrosine. This isotopic exchange reaction was realized in water at 95 ºC in about 30 min. Then, water was evaporated to dryness and it was solved in water again. In this way, the ioiodination yield was found to be about 90 - 95 %.

Speaker: Mrs Gözde Sarican (Ege University, Faculty of Science, Department of Chemistry, Division of Nuclear Chemistry, Bornova, Izmir 35100, Turkey)

Paper ID_162_5_Gözde_Tyrosine_(Full_paper).doc ID_162_5_Gözde_Tyrosine__Full_paper_.pdf

148 Radiolabeling of insuline with fluorine-18 using a new radiofluorination technique

As is known well, insulin is a very important hormone in the body and in case of its absent or its level in the blood is low, glucose is not taken up by most body cells and the body begins to use fat as an energy source. As its level is a central metabolic control mechanism, its status is also used as a control signal to other body systems. For this reason, the sensitively measurement of insulin level in the body is a very important tool in insulin related studies. On the other hand, insulin improves tumor uptake of 2-fluoro-2-deoxy-D-glucose radiolabeled with 18F (18FDG) and its role in diabetic rats with mammary carcinoma was reported in literature. In this context, insulin was earlier labeled by different radionuclides such as 111In, 125I, 18F. It should be also noted that radiolabed form of insulin has expressed the same activity of original insulin in the metabolism. In this study, we have tried to label insulin by using an easier and faster radiofluorination technique. For this, SelectfluorTM has been tried first to be labeled with 18F, then it was used to label insulin. The radiofluorination yield of insuline was found very satisfied.

Speaker: Mrs Cigdem Cetin (Ege University, Faculty of Sciences, Department of Chemistry, Division of Nuclear Chemistry, Bornova, Izmir 35100, Turkey)

Paper ID_161_4_Çiğdem_Insulin_(Full_paper)_2.doc ID_161_4_Çiğdem_Insulin__Full_paper__2.pdf

149 Radiolabelling of nanoparticles for life-cycle studies

An increasing number of products containing engineered nanoparticles (NP) raises the question of potential impacts of the applied NP on the environment. During production, application and final disposal, NP-containing products undergo multiple physical (e.g. abrasion) and chemical (e.g. weathering) processes, that potentially influence and alter the availability and mobility of NP. Crucial factors for the fate of NP in the environment are the degree of particle release from materials as well as the degradability/modification and transport behavior. The investigation of these processes requires experimental tools for extremely sensitive particle tracking. Radiolabelling of NP enables a highly sensitive detection in on-line and in-situ experiments and allows to distinguish sub-processes within complex interactions. It is essential for the application of radiolabelled NP in experimental studies that the radiolabelling process does not alter particle properties and that the radioactive labelling remains stable within the chemical milieu of the experimental setup. Therefore, the use of radioactive basic material for NP-synthesis might be the most appropriate radiolabelling method. However, in some cases the investigation of commercially available NP is required to represent the original properties of the materials used in industrial products. This study presents a method for the radiolabelling of Ag0-NP and TiO2-NP. The radiolabelling was done with 110mAg and 44Ti/45Ti, respectively. Labelling yields, stability tests and comparative NP-characterization are presented.

Speaker: Dr Karsten Franke (HZDR)

150 Radiological dose assessment of naturally occurring radioactive materials in concrete building materials

Previous studies have shown that the natural radioactivity contained in the building material was significantly influenced the dose rates in dwelling. Exposure to natural radiation in building has become more important since almost 80% of our daily live are spend indoor. Thus, the aim of the study is to assess the radiological risk associated with natural radioactivity in soil based building materials to dwellers. A total of 13 Portland cement, 46 sand and 43 gravel samples were obtained throughout the Peninsular of Malaysia and were analysed for their radioactivity concentrations. The activity concentration of 226Ra, 232Th and 40K in the studied building materials samples were found to be in the range of 3.7 Bq kg-1 to 359.3 Bq kg-1, 2.0 Bq kg-1 to 370.8 Bq kg-1 and 10.3 Bq kg-1 to 1949.5 Bq kg-1 respectively. The activity concentration of 226Ra, 232Th and 40K found in the studied building material samples were used to calculate the annual radiation dose rates (μSv year-1) received by dwellers for 1 to 50 years of exposure using Resrad-Build Computer Code. The rooms modelling were based on the changing parameters of concrete wall thickness and the room dimensions. The annual radiation dose rates to dwellers were found to increase annually over a period of 50 years. The dose rate in building was significantly influenced by the thickness of the concrete. The self-absorption occurred when the concrete thickness was higher than 0.4 m. Results of this study show that the dose rates received by the dwellers of the building were proportional to the dimension of the room. In general the study concludes that studied concrete building materials in Peninsular of Malaysia does not pose radiological hazard to the building dwellers since the evaluated dose rates were lower than the recommended limit of 1500 μSv year-1 for building materials. Keywords: Natural radioactivity; Dose rate; Building materials; Resrad-Build Computer Code.

Speaker: Prof. amran majid (universiti kebangsaan malaysia)

151 Radiometric enzyme assays for iodothyronine deiodinases

Details of newly elaborated radiometric methods for extremely sensitive determination of enzyme activities of iodothyronine deiodinases (IDs) of types 1, 2 and 3 are described. IDs catalyze selective 5’- (outer ring) and 5- (inner ring) monodeiodinations of iodothyronines and play crucial roles in the biotransformations of thyroid hormones (TH). Our novel radiometric assays for IDs are based on the use of appropriate high-specific-radioactivity 125I-labeled iodothyronines as substrates; optimized TLC separation of radioactive products from the unconsumed substrates; film-less autoradiography of radio-chromatograms using storage phosphor screens; and quantification of the separated compounds with a BAS-5000 (Fujifilm Life Science Co.) laser scanner. During the developmental process, we found out optimum assay conditions, including concentrations of the respective radioactively labeled substrates; appropriate concentrations of thiol cofactor; the amount of total protein and enzyme concentration in the incubation mixtures; and suitable incubation times for the proper measurement of the individual IDs activities. This methodology enabled us to determine IDs enzyme activities as low as 10 exp -18 katals, in microsomal fractions of different rat and human tissues, as well as in homogenates of cultured mammalian cells. We demonstrated the applicability of our sophisticated radiometric methods by following the alterations of IDs activities induced in cultured rat astroglial cells by a series of purinergic agonists, retinoic acid, and their combination. In the case of ATP as a representative of purinergic agonists, we determined also time-course and dose-response curves to characterize in more details the induction of each type of deiodinase by purines. This work was supported by the Academy of Sciences of the Czech Rep. (Research project No. AV0Z50110509), by the Ministry of Education of the Czech Rep. (Research project No. MSM0021622413), and by the Czech Science Foundation (Grant No. 304/08/0256).

Speaker: Stanislav Pavelka (1Department of Radiometry, Institute of Physiology, Academy of Sciences of the Czech Republic, Prague and 2Central-European Technology Institute, Masaryk University, Brno, Czech Republic)

Poster Sicily113-P-IDs+Pur.pdf

152 Rare earth elements in phosphogypsum and phosphate fertilizers in Brazil

The Brazilian phosphate fertilizers are obtained by wet reaction of the igneous phosphate rock with concentrated sulphuric acid, giving as final product phosphoric acid and dehydrated calcium sulphate (phosphogypsum - PG) as by-product. The level of impurities (metals and radionuclides, among others) present in the phosphate rock used as raw material is distributed among products and by-products. In Brazil, PG has been used for many years in agriculture as a soil amendment. The characterization of natural radionuclides and heavy metals in PG has been extensively studied by several authors. In this paper, the concentration of rare earth elements - REE (Ce, Eu, La, Lu, Nd, Sm, Tb and Yb) present in Brazilian phosphogypsum and the most used phosphate fertilizers (single super phosphate (SSP), triple super phosphate (TSP), monoammonium phosphate (MAP) and diammonium phosphate (DAP)) were determined by instrumental neutron activation analysis - INAA. In order to evaluate the availability of these elements to the soil and plants, the PG samples were extracted with water and a solution of EDTA- NH4 0.05M (procedure established by the European Community) and the REE in the leachate were determined by INAA. REEs concentrate preferentially in PG and the fertilizers TSP and SSP. The results obtained using the methodology with mild leaching of PG with EDTA and total dissolution in water showed that the REEs are not extracted from the PG, and therefore are not available to the environment.

Speaker: Dr Barbara Paci Mazzilli (Instituto de Pesquisas Energeticas e Nucleares)

Paper ID_76_Mazzilli.doc ID_76_Mazzilli.pdf

Poster Poster_INCC_versão_final.pdf

153 Reactor Production of Cu-64 by (n,p) reactions on Zn targets in Dhruva Research Reactor for radiopharmaceutical studies

64Cu is an unique radionuclide, as it undergoes transmutation through three different routes, namely, electron capture (41%), - (40%) and positron emission (19%), and hence is suitable for both PET imaging and targeted therapy. The high specific activity ‘no carrier added’ (N.C.A) grade 64Cu producible from (n,p) reactions on Zn target in medium flux nuclear reactor, is an attractive option to avail the radionuclide, for studies requiring high specific activity product. N.C.A grade 64Cu was produced by neutron irradiation of 1 g zinc foil target (48.63% in 64Zn) sealed in Cadmium shield and encapsulated in standard aluminum container at a neutron flux of ~5.6×1013 n.cm-2.s-1 for 3 days. Irradiated Zn foil was dissolved in 5ml 10M HCl inside a 100 mm thick lead-shielded processing facility with provisions for remote handling. The concentration of resultant clear solution was adjusted to 0.1M with respect to HCl and 1% Ascorbic acid was added to it. The solution was passed through an anion exchange column (Dowex 1×8; 50-100 mesh). 64Cu is retained on the column while the bulk Zn is washed off. Further after washing the column free of ascorbic acid and radioactive Zn, 64Cu is eluted out using a mixture of 3M HCl and H2O2 solution as eluent. The eluate fraction collected was heated to expel H2O2 and reduce the volume. 64Cu radioactivity content and its radionuclide purity were ascertained by -ray spectrometry using HPGe detector coupled to a 4K multichannel analyser system (MCA). Appropriately diluted aliquots of the processed 64CuCl2 solution were measured for 1h, for this purpose. The 1345 keV characteristic photopeak of 64Cu and 511 keV annihilation peak were recorded in the gamma spectra. Radioactivity measured from various batches produced, yielded comparable activity at the end of irradiation. Under the stated conditions of irradiation, 185 MBq 64Cu was separated from solution containing 1 g Zn. Radionuclide purity of greater than 99.9% was achieved through radiochemical separations. Separated 64Cu was evaluated by labeling with MIBI and DOTA ligands. Labeling efficiency of 99.9% was achieved with MIBI and bio-evaluations in mice showed approximately 4-5% uptake in myocardium. However, large uptake in liver and kidneys were also seen for 64Cu-MIBI, which necessitates further studies to explore if any suitable 64Cu complexes for myocardial studies could be identified.

Speaker: Mr vimalnath nair (Bhabha Atomic Research Centre)

154 Relationship between size distribution of radiation-induced aerosol particles and the deposited energy to the air in high-energy proton irradiation.

High-energy proton accelerator produces radiation which induces radiation-chemical reactions of the air in accelerator rooms. The radiolytic product, such as nitrogen oxide, in the accelerator room air forms a huge amount of aerosol particles. In this work, an air chamber was bombarded with a 50-MeV proton beam, and the number concentration and the size distribution of the particles formed in the chamber were measured. Irradiated air was aerosol-free pure air (N2 80%, O2 20%). The beam current, irradiation duration and relative humidity of the air were controlled precisely during the irradiation. The number concentration and geometric mean diameter were found to depend on the beam current which indicated deposited energy to the air. The larger energy was deposited, the larger size and amount of particles were formed. The smallest size of the observed particles was 8 nm in geometric mean diameter. One particle formation required the deposited energy of 15 MeV/cm3. The measurement indicated the formation of the particles had the threshold energy. In the beginning of the irradiation in the aerosol-free air, the radiolytic product is used to form the particles; however, after the formation of the particles the product was mainly consumed in the growth of the particles. The total volume of all particles had a linear relationship with the deposited energy.

Speaker: Mr Naoyuki OSADA (Graduate school of Engineering, Kyoto University)

Paper ID_180_proceedings_20110916_OSADA.doc ID_180_proceedings_20110916_OSADA.pdf

155 Separation of Cu-61 from alpha particle irradiated cobalt target by LLX

Amongst the various radioisotopes available or becoming available for application in nuclear medicine, 61Cu offers an appropriate selection for imaging and targeted radionuclide therapy, due to its superior nuclear properties including desirable half-life and ease of production. Earlier few methods were reported for separation and extraction of 64Cu using various analytical techniques. In this paper, we have attempted to develop a new separation method of no-carrier-added 61Cu from α-irradiated cobalt target. A pure cobalt foil of 21.2 mg/cm2 thickness was irradiated for 12 h with 30 MeV α-particle beam obtained from Variable Energy Cyclotron Centre (VECC), Kolkata, India with an average current 3 µA. The measurements of the activity of radionuclides were done by CANBERRA portable type HPGe detector of 1.9 keV resolutions at 1.33 MeV in conjugation with digital spectrum analyser (DSA 1000) and Genie 2000 software. A stock solution was prepared by dissolving the irradiated target material in 1:1 HNO3,,evaporated to dryness and finally dissolved it 0.01 M HCl. 60Co was spiked into the stock solution. Trioctylamine (TOA) was used as a liquid anion exchanger. In order to study the separation profile, 200 µL stock solution were added to 4 mL HCl of varying strength and was shaken for 10 min with the help of mechanical shaker with equal volume of 0.1 M TOA dissolved in cyclohexane. It was found that at 0.5 M TOA and 3 M HCl, 80% 61Cu was extracted into the organic phase with 25% contamination of bulk cobalt. Copper forms anionic complex [CuCl2]- and [CuCl4]2- which were responsible for preferable extraction of copper into the organic phase. The slight extraction of cobalt might be due to the formation of [CoCl4]- complex. However, the complete decontamination of cobalt is necessary, the study is on progress.

Speaker: Prof. Susanta Lahiri (Saha Institute of Nuclear Physics)

156 Separation of Ra, Ba and Pb for determination of Ra-226 by isotope dilution alpha spectrometry and Pb-210 by liquid scintillation spectrometry

The determination of 226Ra and 210Pb is important for characterization of new and existing reference materials, for use as natural tracers in environmental studies and in environmental assessments when natural radionuclides are present at elevated levels. The 226Ra and 210Pb ratio of characterized reference materials changes with time. Due to possible partial escape of 222Rn from the containers, the calculation of radioactive decay and ingrowth is not reliable after some years, therefore the values have to be re-measured from time to time. In addition soil and sediment matrices usually contain Ba around 100-1000 mg kg-1. This barium content of the samples often disturbs the preparation of the Ra alpha sources and restricts the sample size. The method presented here is based on a simple but efficient separation of Pb and Ra from Ba. After the chemical separation 226Ra is determined by isotope dilution alpha spectrometry (typical resolution of226Ra alpha sources is 30-60 keV FWHM) and 210Pb by liquid scintillation spectrometry. The method is selective and sensitive and provides reliable determination of 226Ra and 210Pb in 0.5-2 g of soil and sediment samples with limits of detectable activities of 0.00016 Bq/sample and 0.006 Bq/sample respectively.

Speaker: Dr Gyula Kis-Benedek (International Atomic Energy Agency (IAEA))

157 Social representation and Nuclear Chemistry educational

Nuclear Chemistry appears very little in high school course curricula or classes in Brazil. This fact hinders students who enroll in higher education without the knowledge necessary for it to exert its full citizenship. This study investigated the public University of São Paulo student´s of understanding of the term "nuclear energy", highlighting the structure of Social Representations (SR). The methodology used was the evocations free from words technique by using the EVOC program, given the frequency in which each element was raised and their average order of evocation to an issue-oriented semantic (cognitive). In this study 124 students were interviewed: from the Chemistry, Pharmacy, Environmental Chemistry, Chemical Engineering and Nutrition Departments (62), Oceanographic Department (29) and Economics, Business Administration and Accounting Department (33). The results indicated that the social representation structure concerning nuclear issues has as its central cognitive element represented by the terms atomic bomb, fission, fusion and radiation. Affective aspects are represented by the terms fear, doubt, worry and curiosity. It was observed that there is a need for educational efforts, and a revision of the educational practices in high school regards to Nuclear Chemistry. The concepts of chemistry and its social factors should be treated in a concrete form in order to demystify erroneous concepts. Reading and educational instruments should be provided to ensure a better understanding of radioactivity phenomena and their applications.

Speaker: Deborah Favaro (Instituto de Pesquisas Energeticas e Nucleares)

Poster Favaro_poster_INCC.pdf

158 Synthesis and characterization of novel asymmetrical M(III) (M = Re, Tc-99g) complexes as models for the development of new potential tracers for SPECT imaging and radiotherapy

Development of new 99mTc and 186/188Re radiopharmaceuticals still remain an interesting research topic thanks to their ideal nuclear properties. 99mTc is the radioisotope of election for SPECT-imaging (Eγ=140 keV, t1/2=6.02 h), and 186/188Re are important radionuclides with therapeutic potential (186Re: Eβ=1.07 MeV, Eγ=137 keV, t1/2=90.6 h; 188Re: Eβ=2.12 MeV, Eγ=155 keV, t1/2=17 h). Despite the rich and diverse coordination chemistry of these two congeners, very few M(III)-complexes are reported in literature and none have clinical applications. Within we report the synthesis and the characterization of a new series of neutral, asymmetrical, hexacoordinated Re/99gTc-complexes of the type [MIII(PS)2(L)] where PS is the strong π-acceptor 2-(dipheny1phosphino)ethanethiolate (PS2) or the completely alkylic non-π-acceptor 2-(diisopropyl)ethanetiolate (PSiso) P,S-bidentate ligands, while L is a dithiocarbamate (DTCn) or pyridine-2-thiolate (MPy) ligands. The [MIII(PS)2(L)] complexes were synthesized starting from precursors where the metal is in different oxidation states, involving ligand exchange reactions and/or reduction-ligand exchange reactions. All the complexes were obtained in moderate to good yield and were found to be diamagnetic, neutral and stable and were characterized by elemental analysis, multinuclear NMR, ESI(+)-QTOF-MS, and cyclic voltammetry. X-ray diffraction analysis was performed on crystallized [ReIII(PS2)2(DTC1)], [ReIII(PS2)2(DTC2)], [99gTcIII(PS2)2(DTC1)] (DTC1 = pyrrolidine-1-carbodithioate; DTC2 = 4-(ethoxycarbonyl)piperidine-1-carbodithioate), and [ReIII(PS2)2(MPy)]. The X-ray structural analysis of [ReIII(PS2)2(DTC1)], [ReIII(PS2)2(DTC2)] and [99gTcIII(PS2)2(DTC1)] revealed for these complexes a distorted octahedral geometry, where the four Sulfur atoms occupy the equatorial plane and the two Phosphorus atoms span the apical positions. [99gTcIII(PS2)2(DTC1)] is isostructural and isomorphic with [Re(PS2)2(DTC1)]. X-rays diffraction data of [ReIII(PS2)2(MPy)] confirm the presence of the pyridine-2-thiolate moiety instead of the MPyO. The collected results indicate the possibility to consider this new class of complexes suitable for the development of novel 99mTc/186/188Re-agents useful in theragnostic applications. Studies are currently in progress in order to transfer this technology at tracer level.

Speaker: Dr Nicolò Morellato (University of Padova, Italy)

159 The production and isolation of Cu-64 after production by the bombardment of a natural Zn target

The production possibility of different copper radionuclides has been investigated by several groups[1-7]. Szelecsényi et al.[8] measured new cross-section data for the 66Zn(p,2pn)64Cu and 68Zn(p,x)64Cu nuclear processes from their respective threshold energies up to 100 MeV and concluded that both processes are suitable for the routine production of 64Cu. A 66Zn target and a 68Zn target can be used, respectively, in the energy windows 70 → 35 MeV and 37 → 10 MeV for the production of 64Cu. At iThemba LABS a natZn target is bombarded with the 66 MeV proton beam for the routine production of 64Cu (and 67Ga). Various methods have been published for the separation of Cu from Zn[1,9-11]. An improved method is presented for the selective purification of Cu radionuclides (specifically 64Cu) from gram amounts of zinc using an ion exchange column containing 5.0 mL XAD-8 which had been impregnated with dithizone (diphenylthiocarbazone). 64Cu was recovered from the 67Ga waste solution which contained ca 8 g Zn. The waste solution was evaporated to dryness and the salts dissolved in 0.05 M HCl (ca pH 2) and passed through the ion exchange column, which had been equilibrated with 0.05 M HCl, Zn was eluted with 0.05 M HCl. Particular attention was paid to the development of optimal elution profiles using respectively 10 M HNO3, 3 M HNO3 and 5 M HCl-1% H2O2. References 1. T. Stoll, S. Kastleiner, Yu. N.Shubin, H.H. Coenen, S.M. Qaim, Radiochim. Acta 90 (2002) 309. 2. F.Szelecsényi, Z. Kovács, T.N van der Walt, G.F. Steyn, K. Suzuki, K. Okada, Appl. Radiat. Isot. 58 (2003) 377. 3. K.Hilgers, T.Stoll, Y. Skakun, H.H Coenen, S.M Qaim, Appl. Radiat. Isot. 59 (2003) 343. 4. M.L. Bonardi, F. Groppi, C. Biratarri, L. Gini, C. Mainardi, A. Ghioni, E. Menapace, K. Abbas, U. Hotzwarth, M.F. Stroosnijder, J. Radioanal. Nucl. Chem. 257 (2003) 229. 5. F. Tárkányi, S. Takács, F. Ditrói, A. Hermanne, M. Sonck, Yu. Subin, Nucl. Instr. and Meth. B 217 (2004) 531. 6. F.Szelecsényi, Z.Kovács, K. Suzuki, K. Okada, T.N van der Walt, G.F. Steyn, S. Mukherjee, J. Radioanal. Nucl. Chem. 263 (2005) 539. 7. M.L. Bonardi, F. Groppi, H.S. Mainardi, V.M. Kokhanyuk, E.V. Lapsina, M.V. Mebel, B.L. Zhuikov, J. Radioanal. Nucl. Chem. 264 (2005) 101. 8. F.Szelecsényi, G.F. Steyn, Z.Kovács, C. Vermeulen, N.P. van der Meulen, S.G. Dolley, T.N van der Walt, K. Suzuki, K. Mukai, Nuclear Instruments and Methods in Physics B 240 (2005) 625. 9. F.W.E. Strelow, Talanta 35 (1988) 385. 10. R. Scharczbach, K. Zimmermann, P. Blauenstein, A. Smith, P.A. Schubiger, Appl. Radiat. Isot. 46 (1995) 329. 11. C. Naidoo, T.N. van der Walt, Appl. Radiat. Isot. 54 (2001) 915.

Speaker: Prof. Tjaart Nicolaas (Nico) van der Walt (Cape Peninsula University of Technology)

160 Total Diet Study: Mg and Mn content estimation of a Market Basket of São Paulo state (Brazil) by Instrumental Neutron Activation.

Total Diet Studies (TDS) have been carried out to estimate dietary intakes of the essential and toxic elements for a large-scale population over a specific period of time. In general, a Market Basket (MB) approach is adopted. In this study, the TDS was based on the evaluation of food representing a MB, which reflected the dietary habits of the São Paulo State population, corresponding to 72% of the average food consumption for the state of São Paulo. In the present TDS, magnesium and manganese concentrations were determined in 30 of the most consumed food groups of a Market Basket of São Paulo State - Brazil. Element concentrations were determined by instrumental neutron activation analysis in freeze-dried samples and the values in the table-ready food groups ranged: Mg 37.9 (beverages) to 450.4 mg/kg (breads) and Mn 0.10 (prime grade beef) to 14.6 mg/kg (flours). The average daily Mg and Mn intakes were calculated by multiplying the concentration of each element in each table-ready food group by the respective weight (g/day) of the food group in the MB and adding the products from all food groups. The results of daily dietary intakes in this study were 90.85 mg Mg day-1 and 1.34 mg Mn day-1. Theses values were lower than the adequate intake (AI) proposed by the Food and Nutrition Board, Institute of Medicine (USA, National Academies) for adults. The low levels of Mg and Mn intakes presented in this TDS are probably due to the fact that MB of this study represented only 72% of the weight of the most consumed household foods of São Paulo State.

Speaker: Dr Vera Akiko Maihara (IPEN-CNEN/SP)

Paper ID_74_MaiharaV.A._Paper.pdf

Poster Poster_Vera_DietaTotal.pdf

161 U, Th and other element evaluation in wild mushroom from a naturally high radioactive region in Brazil

Mushrooms are fungi species which have high capacity to retain elements and radionuclides such as 137Cs, 238U, 232Th, from the environment. Studies have demonstrated that wild mushrooms can be used as environmental indicators and monitors to evaluate contamination and quality of ecosystems. Several studies have determined a high level of radionuclide in agricultural products in the Poços de Caldas region, which has seventy, identified radiological anomalies. The present study, which aimed at U, Th, As, La, Fe, Zn, Se, Cr, Cs, Co, Rb, and Sc bioaccumulation mushroom capacity, was based on the determination of these elements content in 15 wild mushroom samples collected in different points from Poços de Caldas Plateau region, without concern to radiological anomalies location. These elements were chosen due to their relative abundance in the Plateau soil. The analytical methodology employed was Instrumental Neutron Activation Analysis. Accuracy and precision of the analyses were verified with IAEA Mushroom Reference Material. The results obtained are discussed considering the geological context of the region and there was a large element level variation among the analyzed mushroom samples. The highest elemental concentrations, mainly of U and Th, occurred in samples collected in rural areas, where most radioactive anomalies are known to be located. Data showed that the wild mushroom can be used as a bio-indicator of the environmental radioactive contamination.

Speaker: Dr Vera Akiko Maihara (IPEN-CNEN/SP)

Paper ID_75_Rosa_M.pdf

Poster POSTER_-_Vera_Mushroom.pdf

Dinner: at San Vito lo Capo - bus included, dinner not included

Friday 23 September

Session 13: Health Physics

162 Radiation protection relevant to Nuclear Chemistry in the light of recent International Recommendations

The paper discusses the requirements for radiation protection in nuclear chemistry which are related to the recent recommendations of the International Commission on Radiological Protection. These recommendations are currently being incorporated into the International Basic Safety Standards to be issued by the International Atomic Energy Agency later this year as well as into new relevant Directives of the European Union based on which the legislature of the Member States have to be updated. New international requirements are aimed at further improvement of strict control of radiation sources, their safety and security as well as the minimization of the exposure to workers and members of the public. These tasks would require not only some changes in national systems of radiation protection and nuclear safety, but also appropriate measures should to be taken to train personnel responsible for the implementation of new regulations in order to achieve compliance with international standards. It would only be appropriate if nuclear chemistry community is familiar with the forthcoming changes in radiation protection well in advance so that it would be easier for nuclear chemists to adopt new requirements in their everyday practical work where they handle various radioactive sources and have to be familiar how to protect themselves and others in line with these new requirements.

Speaker: Dr Jozef Sabol (Czech Technical University, Faculty of Biomedical Engineering)

Paper ID_154_Sabol,_Radiation_protection_relevant_to_Nuclear_Chemistry,_.docx ID_154_Sabol,_Radiation_protection_relevant_to_Nuclear_Chemistry,_p.pdf

163 TENORM accumulation and management in refineries

Naturally occurring radionuclides are present at varying concentrations in the Earth’s crust and can be concentrated by processes associated with various industrial activities, such as the ones involved in the recovery of oil and gas. This “enhanced” NORM (Naturally Occurring Radioactive Material) are also known as TENORM (Technologically Enhanced NORM) and their presence in the upstream oil sector is a widely known phenomenon, that occurs because of the large quantities of production water usually present in the plants, that can carry up to the surface the radium-226 and radium-228 salts that form in the reservoir. In production plant therefore there might be presence of large amounts of TENORM in the form of sludge, scale, mud, etc, with varying activity concentration and usually large presence of radium-226 and radium-228. In the downstream oil sector, nevertheless, water percentage upon the total product (watercut) is usually very low, thus lacking the main reason of NORM presence in components for upstream sector. In this work, it is presented eni’s 4-step plan for the evaluation of TENORM presence in refineries, its characterization and the management of the risk coming from its presence. The first step of the plan is a preliminary survey in various refineries, to detect the presence of radiometric anomalies on components caused by TENORM, comprising the collection of samples of different matrixes, potentially contaminated by natural radionuclides. Dose rate values higher than environmental background were detected in some areas of the plants, i.e. the mud treatment area, the water storage tank, desalters, the cocking heater, the crude storage tank. Samples collected from these points showed increased concentrations of natural radionuclide, especially lead-210 concentration up to 15000 Bq/kg, to be compared to radium-226 activity concentration not exceeding 200 Bq/kg. Since TENORM are present at all, it was necessary to evaluate the exposure of the workers of the plant and to check that it is compliant to Italian Legislation dose limit, equal to 1 mSv/annum. To perform the dose assessment, working activities are divided into 2 main categories, ordinary activities that include plant surveillance and parameters registration, and extra-ordinary maintenance such as components cleaning, maintenance and decommissioning. Next stage is the workers training, based on a general radioactivity induction and information about the risk of the specific site. Eni also introduced contaminated components labelling with dedicated signals. Finally, all the waste coming from these plants should be adequately sampled and characterized, to assure best disposal solution depending of their radiometric content.

Speaker: Dr Enrico Rizzio (eni S.p.A. Exploration & Production Division)

Paper

• ID_195_TENORM_Accumulation_and_Management_in_refineries_-_Rizzio.doc
• ID_195_TENORM_Accumulation_and_Management_in_refineries_-_Rizzio.doc
• ID_195_TENORM_Accumulation_and_Management_in_refineries_-_Rizzio.pdf

164 Decontamination of radioactive concrete in nuclear facilities by chemical separation method.

Europium and cobalt etc., contained in the biological shield concrete, are made a radiation with the neutron during the nuclear power plant and the accelerator facilities in operation. At the end of operation, biological shield concrete may be considered as radioactive wastes due to these radioactive nuclides. However, it is thought europium and cobalt content in the biological shield concrete is very little, thus trace amount of the radionuclide determined entire biological shield concrete as radio waste and the handling cost is severe. Therefore, the introduction of chemical processing, and the possibility of a significant amount of waste volume reduction had been found.

Speakers: Dr Shun Sekimoto (Kyoto University), Mr Yuichi Tanimoto (Shimizu Corporation)

165 Assessment of dose to the Irish population arising from anthropogenic radioactivity in the Irish marine environment

Since the early 1980’s the Radiological Protection Instiute of Ireland (RPII) has carried out extensive monitoring of the levels of anthropogenic radioactivity in the Irish marine environment through analysis of fish, shellfish, seaweed and sediment samples. The most significant source of this anthropogenic radioactivity arises from the liquid discharges from the Sellafield nuclear reprocessing plant located in the Eastern Irish sea and the radionuclides of primary interest are Cs-137, Tc-99, Pu-238 and Pu-239,240. The RPII has always used the results from the marine monitoring programme to assess the dose arising from consumption of fish and shellfish. Recent work carried out by the RPII and Centre for Environment, Fisheries and Aquaculture Science (CEFAS) has identified other critical exposure pathways that would need to be assessed in order to obtain a more comprehensive dose assessment for members of the public. These pathways include ingestion of seaweed, inhalation of seaspray, external exposure arising from exposure to beach sediments and, to a lesser extent, occupational exposure through handling of fishing equipment. This work assesses the dose arising from all of these pathways using the European Commission CREAM methodology in conjunction with data from the RPII’s monitoring programme and habits data of the Irish population and identifies the critical exposure pathways and the radionuclides of primary concern from a dose assessment perspective.

Speaker: Mr Kevin Kelleher (Radiological Protection Instiute of Ireland)

Paper ID_5_Kelleher.doc ID_5_Kelleher.pdf

166 Measurements of the spatial distribution of each dose component in tissue exposed to an epithermal neutron beam for BNCT

In tissue exposed to high-flux epithermal neutron beams, the reactions mainly responsible for the absorbed dose in tissue are those with hydrogen and nitrogen, that is 1H(n,γ)2H (σ = 0.33 b), whose γ-rays of 2.2 MeV can travel many centimetres through tissue, and 14N(n,p)14C (σ = 1.81 b), whose emitted protons of about 0.6 MeV have short range in tissue, giving local dose deposition. The fast neutron component of epithermal neutron beams, gives a not negligible contribution to the absorbed dose mainly due to elastic scattering with hydrogen nuclei. If the isotope 10B is selectively accumulated in tumour tissue, the reaction with thermal neutrons 10B(n,α)7Li (σ = 3837 b) causes localised energy absorption in cancerous cells; this is exploited by boron neutron capture therapy (BNCT). It is mandatory to separate the various dose contributions, owing to their different biological effectiveness. The dosimetry method based on Fricke-Xylenol-Orange-infused gels in form of layers has shown noticeable potentiality for in-phantom or in-free-beam dose distribution measurements in the high fluxes of thermal or epithermal neutrons. In fact, a method has been developed that gives the possibility of obtaining the spatial distribution of each dose component. The discrimination of the various dose contributions is achieved by means of pixel-to-pixel manipulations, with suitable algorithms, of pairs of dose images obtained with gel-dosimeters having different isotopic composition. It is possible to place large dosimeters, detecting in such a way large dose images, because the layer geometry of dosimeters avoids sensitive variation of neutron transport due to the gel isotopic composition. Various measurements, both in phantom and in free-beam, have been carried out at the collimator of the epithermal column of the LVR-15 research reactor in Řež (CZ), which is suitably designed for BNCT treatments.

Speaker: Prof. Grazia Gambarini (Università degli Studi di Milano and INFN, Milano, Italy)

10:30 coffee break

Session 14: Radioanalytical Chemistry and Nanoparticles

167 Simultaneous speciation analysis of arsenic, antimony and selenium in natural waters by HPLC, SPE and solvent extraction coupled to neutron activation

Simultaneous speciation neutron activation analysis (SSNAA) technique is being developed in our laboratory over the last 20 years or so. This technique can be reliably used for the simultaneous determination of not only various species of a single element but also species of other elements present in the same sample. Almost all speciation techniques consist of two steps. The first step involves the separation of species from the sample followed by the second step of element-specific detection. A neutron activation analysis (NAA) method in combination with high-performance liquid chromatography (HPLC) was developed first for the determination of low levels of five arsenic species, namely As(III), As(V), monomethylarsonic acid (MMA), dimethylarsinic acid (DMA), and arsenobetaine (AsB) in water samples. Organically bound arsenic (OBAs) and total arsenic levels were also measured. The detection limits of the HPLC-NAA method were found to be between 0.005 and 0.12 ng/mL for OBAs and total arsenic, respectively, using the Dalhousie University SLOWPOKE-2 reactor facility. These methods were then extended to include the determination of arsenic, antimony and selenium species, namely As(III), As(V), Sb(III), Sb(V), and Se(IV), in natural water samples by solvent extraction using APDC/MIBK and by solid-phase extraction (SPE) using HDBDC/XAD-4. Details of all three methods will be presented along with the concentrations of various species measured in natural waters.

Speaker: Prof. Amares Chatt (SLOWPOKE-2 Facility, Trace Analysis Research Centre, Department of Chemistry, Dalhousie University, Halifax, NS, B3H 4J3, Canada)

Paper Shi_Chatt_INCC-3_AsSbSe_2013_08_11_F1.doc Shi_Chatt_INCC-3_AsSbSe_2013_08_11_F1.pdf

168 The present role of radiochemical neutron activation analysis (RNAA) for determination of essential and toxic trace elements in biological materials as–compared with ICP-MS and AAS

There is a need for reliable determination of low levels of essential elements in human, animal and plant tissues, as well as for elements, which are toxic to organisms at trace concentrations. The former category of essential elements comprises B, Co, Cr, Cu, F, Fe, I, Mn, Mo, Ni, Se, Si and Zn (sometimes, depending upon the definition Li and V are added to this list), while in the latter category the toxic metals As, Cd, Hg, Pb and Tl are mostly mentioned (additionally Be, Sb and organic Sn compounds may also be considered in this category). For low-level determination of the elements As, Cd, Co, Cr, Cu, Hg, I, Mo, Ni, Sb, Se, Si, Sn, Tl various RNAA procedures were developed over the years, which frequently provided a unique possibility of determination of the above elements. Highly competitive bulk sample analytical techniques, namely various modes of AAS and ICP-MS have been developed in the last decades. Nowadays, these techniques surpassed RNAA not only in the usage frequency (which has never been a precedence of RNAA), but also in other performance characteristics. Nevertheless, there are still unique features of RNAA, such as its essentially blank-free nature, high specificity, the possibility of the chemical yield determination that yield high accuracy and low uncertainty of determination of selected elements at extremely low levels and make this technique viable and indispensable in various application fields. This paper presents a comparison of selected RNAA procedures with AAS and ICP-MS methods for most of the above elements. It aims at identification of possibilities and limitations of these techniques and applications in which RNAA should be considered a premier analytical technique for trace element analysis of biological materials. Future trends in RNAA are also outlined.

Speaker: Prof. Jan Kucera (Nuclear Physics Institute ASCR, Rez, Czech Republic)

169 Ultra sensitive measurements of Th-232 in copper by RNAA

Copper, thanks to its low content in radioactive contaminations, is a material widely used for shields, holders and others objects close to sensitive parts of the detectors in many experiments on Rare Events Physics. This imply that tools able to reach sensitivity of the order of <10-12 g of contaminants / g of Copper are of crucial importance. A methodology based on Neutron Activation Analysis (NAA) has been developed to obtain an extremely high sensitivity in the analysis of 232Th in Copper samples. A detection limits of 5 x 10-13 g 232Th /g Cu have been achieved through the irradiation of 200 g of copper sample which subsequently was been radiochemical concentrated using Nitric Acids and then Actinide Resin from Eichrom Inc. Several elutions with various inorganic acids were done to concentrate the 232Th activation product (233Pa) from copper matrix and to also eliminate the radioactive background induced by the neutron bombardment to reach an higher sensitivity.

Speakers: Dr Andrea Salvini (Università di Pavia), Dr Massimiliano Clemenza (Università di Milano Bicocca)

170 Total and bioaccessible fractions of trace elements in cultivated oyster tissues by INAA, PIXE and ICP-MS

Estimation of the total and bioaccessible fraction of both nutritionally and toxicologically important elements in cultivated oysters consumed by Japanese population groups are of much interest. Oysters are cultivated in Japan by hanging them on an 11-m long rope in the ocean. Levels of 20 elements in these oysters were investigated. Three bunches of oyster were collected at 1, 6, and 11 m depths. From each bunch, five oysters were chosen, washed with tap water, and removed from the shell. Two groups of organ, namely (i) hepatopancreas and muscle, and (ii) gill and mantle, were separated from soft tissues, freeze-dried, and pulverized. One portion of it was irradiated at the Dalhousie University SLOWPOKE-2 reactor facility in Halifax, Canada for assaying Ag, Br, Cl, Cu, Mg, Na, Se, and V by instrumental neutron activation analysis (INAA) through their short- and medium-lived nuclides. Another portion was irradiated at the Kyoto University Reactor in Osaka, Japan for Co, Cr, I, Fe, Rb, Sc, and Zn by INAA using mostly long-lived nuclides. A third portion of the sample was digested in a microwave oven with nitric acid and analyzed for more than 20 elements by particle induced X-ray emission (PIXE). Almost all elements except Cd, Cl, and Ni were found to accumulate in soft tissues with increasing depth. The bioaccessible fraction of the elements was estimated by an in vitro enzymolysis method followed by ICP-MS. Details of experiments and results will be presented.

Speaker: Dr Michiko Fukushima (Ishinomaki Senshu University)

171 Determination of Tc-99 in seaweed sample by ICP-MS

Due to its high mobility, no stable isotope and long half-life (2.1×105 y), 99Tc is one of the most important radionuclide in safety assessment of radioactivity in environment as well as nuclear waste management. Because of the high enrichment of 99Tc in seaweed, it is widely used as a bioindicator for the marine research using 99Tc. These works require a rapid and accurate method for the sensitive determination of 99Tc in various environmental materials. Because of the volatile property and low concentration in the environment, the chemical separation and purification of Tc is the most critical step for the accurate determination of 99Tc. Here, we present an analytical method for 99Tc in seaweed sample. The analytical procedure includes four steps: (1) sample ash and 99Tc leaching, (2) co-precipitation pre-concentration of 99Tc, (3) Removal interferences mainly Mo and Ru, and (4) ICP-MS detection of 99Tc. 99mTc was used as a yield monitor to check the loss of 99Tc in each step. It was observed that the organic matrix of seaweed samples can be incinerated completely at 700 0C in 3h without significant loss of Tc. For Mo and Ru decontamination, extraction chromatography using TEVA resin was applied and a sufficiently high decontamination factors for Mo and Ru have been obtained in this work. The separated 99Tc in the eluate from the chromatograph was measured by ICP-MS with lower detection limit after one week decay of 99mTc. The total chemical yield of Tc in whole procedure is above 85% and analysis of a batch of samples (8-12) can be completed within 12h. The procedure was proved to be reliable and can be used in the environmental sample`s analysis by analyzing some standard reference materials.

Speakers: Keliang Shi (Risø National Lab for Sustainable Energy, Technical University of Denmark, DK-4000 Roskilde, Denmark), Xiaolin Hou (Risø National Lab for Sustainable Energy, Technical University of Denmark, DK-4000 Roskilde, Denmark)

172 A nuclear measurement technique for comparison of the washing machine detergent qualities used on the market

Many washing machine detergents with different marks can easily found on the market. In this study, we have investigated the cleaning qualities of the washing machine detergents which are used in homes applying a nuclear measurement technique. Small tissue pieces (3 x 3 cm) made in cotton, have been used as a reference material which is commonly used by individuals or by related commercial companies. For measurement and comparison of cleaning qualities of the washing machine detergents, the tissue pieces were first contaminated plunging into the MIBI complex of 99mTc radioactivity and waited about 30 min. Then, the tissue pieces were washed two times with pure water. It was clearly observed that the 99mTc radioactivity has strongly incorporated into the structure of tissue pieces and could not be practically more removed from the tissue pieces by additional washing with pure water. Then, the tissue pieces were separately immersed into the different mark of diluted aqueous detergent solutions obtained heating to boiling point, waited 15 min, dried by a hair drier machine, and counted in a well NaI(Tl) detector counting system. Finally, it was observed that the detergents with different marks which are sold on the market expressed different cleaning qualities under the same experimental conditions applied in this study. We believe that this kind of quality measurement technique of washing machine detergents applying a nuclear measurement technique was first applied in the literature and this technique is, of course, very sensible respecting to other probable classical techniques applied in this sector. For this reason, we recommend this measurement technique to the detergent manufacturers for testing the quality controls of their products before to place on sale on the markets. It is also very interesting to note that the detergent qualities were not really correlated with their market prices.

Speaker: Mrs Selen Ekim (Ege University)

Paper ID_149_6_Selen_Detergent_(Full_paper).doc ID_149_6_Selen_Detergent__Full_paper_.pdf

13:00 Lunch

Poster Winners Award & Closing Cerimony