Speaker
Description
Interpreting the operating history of a nuclear reactor is a key question in safeguards, non-proliferation, and studies of environmental contamination. It can help answer questions related to the amount and quality of Pu or other radioactive materials that were produced during the irradiation. Traditional approaches to characterizing spent nuclear fuels rely either on radiometric counting and/or mass spectrometry, usually relying on chemical purification of the specific analyte to increase precision and accuracy. Here we present an approach using resonance ionization mass spectrometry (RIMS) to precisely analyze small, solid samples of spent nuclear materials to characterize isotope ratios of multiple elements simultaneously, without prior chemical separation. Dispensing with chemical separation avoids the addition of chemistry “blanks” (background), measuring multiple elements from the same volume allows the correlation of multiple irradiation characteristics, and working from small samples decreases the radioactive hazards in the laboratory.
We have applied Lawrence Livermore National Laboratory’s Laser Ionization of Neutrals (LION) instrument [1] to several samples of spent nuclear material (see Figure 1). This presentation will explain how we can analyze nearly any combination of 3 elements including U, Pu, Am, Sr, Rb, Mo, Zr, Nd, Ba, Cs simultaneously [2], during a single measurement, usually with enough material remaining to analyze the others in a subsequent analysis. We will show how connecting multiple isotope ratios across elements and comparing those analytical results to computational models provide an improved understanding of the operating history of a nuclear reactor.
References:
[1] Savina, M.R., Isselhardt, B.H., Trappitsch, R., “Simultaneous Isotopic Analysis of U, Pu, and Am in Spent Nuclear Fuel by RIMS”, Anal. Chem., doi.org/10.1021/acs.analchem.1c01360, (2021).
[2] Savina, M.R., Isselhardt, B.H., Shulaker, D.Z., Robel, M., Conant, A.J., and Ade, B.J., “Fission products in spent nuclear fuel particles: Simultaneous Sr, Mo, and Ru isotopic analysis by Resonance Ionization Mass Spectrometry”, Sci. Rep., 13, no. 1 (2023): 5193, (2023).
This work performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. LLNL-ABS-843771.
| Workshop Themes | Sample analysis and standards |
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