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Title: Molybdenum isotope compositions of uranium ore concentrates by double spike MC-ICP-MS

Abstract

The molybdenum (Mo) isotope composition of uranium ore concentrate (UOC) has been proposed as a nuclear forensic signature due to the ubiquitous presence of Mo in the nuclear fuel cycle and to the possibility that different UOC production pathways lead to characteristic Mo isotope fractionation. Furthermore, Mo forms a volatile hexafluoride which leads to the retainment of Mo in the nuclear fuel cycle through U enrichment and reactor operation processes. As a result, it is possible that the nuclear fuel cycle generates a rich array of Mo isotope signatures. The first step in interpreting Mo isotope signatures generated during the nuclear fuel cycle is to characterize the Mo isotope composition of starting materials. In this study, a suite of UOC samples were analyzed for their Mo isotope composition in order to constrain the range of Mo isotope compositions entering the front end of the nuclear fuel cycle. Analytical protocols were developed to purify Mo from a U rich matrix prior to Mo isotope analysis by double spike MC-ICP-MS. A >3‰ variation in the 98Mo/ 95Mo ratio was observed in the suite of UOC samples with δ 98Mo ranging from -1.15 to +1.96‰ relative to the NIST 3134 Mo standard referencemore » material. The δ98Mo range observed in the UOC samples is very similar to the δ 98Mo range observed in crustal igneous rocks and Mo-bearing minerals, suggesting that Mo isotope variability in UOC is driven by variability in the parent U ores. However, Mo isotope fractionation during UOC production is evident with one of the UOC samples being isotopically heavy relative to its parent U ore by 0.75‰, suggesting that different UOC production processes also contribute to the total Mo isotope variability observed. Overall, it is expected that the Mo isotope signatures generated during enrichment and reactor process will be clearly discernible from those generated during UOC production.« less

Authors:
 [1];  [2];  [3];  [4];  [1];  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Nuclear and Chemical Sciences Division, Physical and Life Sciences Directorate
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Nuclear and Chemical Sciences Division, Physical and Life Sciences Directorate; Univ. of Otago, Dunedin (New Zealand). Dept. of Chemistry and Centre for Trace Element Analysis
  3. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Nuclear and Chemical Sciences Division, Physical and Life Sciences Directorate; Univ. of Munster, Munster (Germany). Inst. fur Planetologie
  4. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Nuclear and Chemical Sciences Division, Physical and Life Sciences Directorate; Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1502043
Report Number(s):
LLNL-JRNL-758218
Journal ID: ISSN 0883-2927; 944136
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Accepted Manuscript
Journal Name:
Applied Geochemistry
Additional Journal Information:
Journal Volume: 103; Journal Issue: C; Journal ID: ISSN 0883-2927
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Citation Formats

Rolison, John M., Druce, Matthew, Shollenberger, Quinn R., Kayzar-Boggs, Theresa M., Lindvall, Rachel E., and Wimpenny, Josh. Molybdenum isotope compositions of uranium ore concentrates by double spike MC-ICP-MS. United States: N. p., 2019. Web. doi:10.1016/j.apgeochem.2019.03.001.
Rolison, John M., Druce, Matthew, Shollenberger, Quinn R., Kayzar-Boggs, Theresa M., Lindvall, Rachel E., & Wimpenny, Josh. Molybdenum isotope compositions of uranium ore concentrates by double spike MC-ICP-MS. United States. doi:10.1016/j.apgeochem.2019.03.001.
Rolison, John M., Druce, Matthew, Shollenberger, Quinn R., Kayzar-Boggs, Theresa M., Lindvall, Rachel E., and Wimpenny, Josh. Mon . "Molybdenum isotope compositions of uranium ore concentrates by double spike MC-ICP-MS". United States. doi:10.1016/j.apgeochem.2019.03.001.
@article{osti_1502043,
title = {Molybdenum isotope compositions of uranium ore concentrates by double spike MC-ICP-MS},
author = {Rolison, John M. and Druce, Matthew and Shollenberger, Quinn R. and Kayzar-Boggs, Theresa M. and Lindvall, Rachel E. and Wimpenny, Josh},
abstractNote = {The molybdenum (Mo) isotope composition of uranium ore concentrate (UOC) has been proposed as a nuclear forensic signature due to the ubiquitous presence of Mo in the nuclear fuel cycle and to the possibility that different UOC production pathways lead to characteristic Mo isotope fractionation. Furthermore, Mo forms a volatile hexafluoride which leads to the retainment of Mo in the nuclear fuel cycle through U enrichment and reactor operation processes. As a result, it is possible that the nuclear fuel cycle generates a rich array of Mo isotope signatures. The first step in interpreting Mo isotope signatures generated during the nuclear fuel cycle is to characterize the Mo isotope composition of starting materials. In this study, a suite of UOC samples were analyzed for their Mo isotope composition in order to constrain the range of Mo isotope compositions entering the front end of the nuclear fuel cycle. Analytical protocols were developed to purify Mo from a U rich matrix prior to Mo isotope analysis by double spike MC-ICP-MS. A >3‰ variation in the 98Mo/95Mo ratio was observed in the suite of UOC samples with δ98Mo ranging from -1.15 to +1.96‰ relative to the NIST 3134 Mo standard reference material. The δ98Mo range observed in the UOC samples is very similar to the δ98Mo range observed in crustal igneous rocks and Mo-bearing minerals, suggesting that Mo isotope variability in UOC is driven by variability in the parent U ores. However, Mo isotope fractionation during UOC production is evident with one of the UOC samples being isotopically heavy relative to its parent U ore by 0.75‰, suggesting that different UOC production processes also contribute to the total Mo isotope variability observed. Overall, it is expected that the Mo isotope signatures generated during enrichment and reactor process will be clearly discernible from those generated during UOC production.},
doi = {10.1016/j.apgeochem.2019.03.001},
journal = {Applied Geochemistry},
number = C,
volume = 103,
place = {United States},
year = {2019},
month = {4}
}

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