A composite position independent monitor of reactor fuel irradiation using Pu, Cs, and Ba isotope ratios

When post-irradiation materials from the nuclear fuel cycle are released to the environment, certain isotopes of actinides and fission products carry signatures of irradiation history that can potentially aid a nuclear forensic investigation into the material's provenance. In this study, combin...

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Bibliographic Details
Published in:Journal of environmental radioactivity 2018-12, Vol.195 (C), p.9-19
Main Authors: Robel, Martin, Isselhardt, Brett, Ramon, Erick, Hayes, Anna, Gaffney, Amy, Borg, Lars, Lindvall, Rachel, Erickson, Anna, Carney, Kevin, Battisti, Terry, Conant, Andrew, Ade, Brian, Trellue, Holly, Weber, Charles
Format: Article
Language:English
Subjects:
Barium isotope ratio
Barium Radioisotopes - analysis
Cesium isotope ratio
Cesium Radioisotopes - analysis
Cesium-133
Cesium-135
Cesium-137
Environmental release
Fission products
Mass Spectrometry
Nuclear forensics
NUCLEAR FUEL CYCLE AND FUEL MATERIALS
Nuclear nonproliferation
Nuclear Reactors
Nuclear safeguards
Nuclear terrorism
Plutonium - analysis
Plutonium isotope ratio
Radiation Monitoring - instrumentation
Reactor modeling
Spent fuel analysis
Stable isotopes
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Summary:When post-irradiation materials from the nuclear fuel cycle are released to the environment, certain isotopes of actinides and fission products carry signatures of irradiation history that can potentially aid a nuclear forensic investigation into the material's provenance. In this study, combinations of Pu, Cs, and Ba isotope ratios that produce position (in the reactor core) independent monitors of irradiation history in spent light water reactor fuel are identified and explored. These position independent monitors (PIMs) are modeled for various irradiation scenarios using automated depletion codes as well as ordinary differential equation solutions to approximate nuclear physics models. Experimental validation was performed using irradiated low enriched uranium oxide fuel from a light water reactor, which was sampled at 8 axial positions from a single rod. Plutonium, barium and cesium were chemically separated and isotope ratio measurements of the separated solutions were made by quadrupole and multi-collector inductively coupled mass spectrometry (Cs and Pu, respectively) and thermal ionization mass spectrometry (Ba). The effect of axial variations in neutron fluence and energy spectrum are evident in the measured isotope ratios. Two versions of a combined Pu and Cs based PIM are developed. A linear PIM model, which can be used to solve for irradiation time is found to work well for natural U fuel with
ISSN:0265-931X
1879-1700
DOI:10.1016/j.jenvrad.2018.08.014