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

Rolison, John M.; Druce, Matthew; Shollenberger, Quinn R.; Kayzar-Boggs, Theresa M.; Lindvall, Rachel E.; Wimpenny, Josh

doi:10.1016/j.apgeochem.2019.03.001

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

Full Record
Other Related Research

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 δ⁹⁸Mo ranging from -1.15 to +1.96‰ relative to the NIST 3134 Mo standard reference material. Themore »« less

Authors:

Rolison, John M. ^[1]; Druce, Matthew ^[2]; Shollenberger, Quinn R. ^[3]; Kayzar-Boggs, Theresa M. ^[4]; Lindvall, Rachel E. ^[1]; Wimpenny, Josh ^[1]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Nuclear and Chemical Sciences Division, Physical and Life Sciences Directorate
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
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
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:: 2019-04-08

Research Org.:: Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1502043

Alternate Identifier(s):: OSTI ID: 1636664

Report Number(s):: LLNL-JRNL-758218
Journal ID: ISSN 0883-2927; 944136

Grant/Contract Number:: AC52-07NA27344; 18-ERD-016

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.

Copy to clipboard


                    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.  https://doi.org/10.1016/j.apgeochem.2019.03.001

Copy to clipboard


                    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.  https://doi.org/10.1016/j.apgeochem.2019.03.001.  https://www.osti.gov/servlets/purl/1502043.

Copy to clipboard


                    
@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}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (Publisher)

Accepted Manuscript (DOE)

Publisher's Version of Record

https://doi.org/10.1016/j.apgeochem.2019.03.001

Other availability

Search WorldCat to find libraries that may hold this journal

Citation Metrics:

Cited by: 14 works

Citation information provided by
Web of Science

Save / Share:

Export Metadata

Save to My Library

Similar Records in DOE PAGES and OSTI.GOV collections:

Samarium isotope compositions of uranium ore concentrates: A novel nuclear forensic signature

Journal Article Shollenberger, Quinn R. ; Borg, Lars E. ; Ramon, Erick C. ; ... - Talanta

Uranium ore is mined and milled to produce uranium ore concentrate (UOC), a regulated product of the nuclear fuel cycle. Additionally, diversion of UOC from the fuel cycle into possible weapons production is a key concern in global nonproliferation efforts. As such, the ability to trace the origin of seized nuclear materials is imperative to law enforcement efforts. Although isotopic signatures of UOCs have proven fruitful to pinpoint sample provenance, new isotopic signatures are needed because most existing isotopic signatures are not indicative of the original ore body from which the U is derived. In this work, we developed amore »« less
https://doi.org/10.1016/j.talanta.2020.121431

Full Text Available
Rare-earth element fractionation in uranium ore and its U(VI) alteration minerals

Journal Article Balboni, Enrica ; Spano, T ; Cook, N ; ... - Applied Geochemistry

We developed a cation exchange chromatography method employing sulfonated polysterene cation resin (DOWEX AG50-X8) in order to separate rare-earth elements (REEs) from uranium-rich materials. The chemical separation scheme is designed to reduce matrix effects and consequently yield enhanced ionization efficiencies for concentration determinations of REEs without significant fractionation using solution mode-inductively coupled plasma mass spectrometry (ICP-MS) analysis. This method was then applied to determine REE abundances in four uraninite (ideally UO₂) samples and their associated U(VI) alteration minerals. In three of the samples analyzed, the concentration of REEs for primary uraninite are higher than those for their corresponding secondary uraniummore »« less
Cited by 16
https://doi.org/10.1016/j.apgeochem.2017.10.007

Full Text Available
Determining provenance of uranium ore concentrates using 143Nd/144Nd

Journal Article Devlin McLoughlin, Victoria E. ; Shollenberger, Quinn R. ; Brennecka, Gregory A. - Talanta

The neodymium (Nd) isotopic composition—particularly ¹⁴³Nd/¹⁴⁴Nd—of a material has long been a source of information utilized in the fields of geochemistry and cosmochemistry due to the radiogenic nature of ¹⁴³Nd. Uranium ore concentrates (UOCs) often contain Nd in measurable quantities, meaning ¹⁴³Nd/¹⁴⁴Nd can also be employed to determine the provenance of regulated nuclear material early in the fuel cycle. Here, we use an improved chemical separation technique and plasma-source multi-collector mass spectrometry to investigate the ¹⁴³Nd/¹⁴⁴Nd compositions of 28 UOC samples. We show that these UOCs exhibit highly variable ¹⁴³Nd/¹⁴⁴Nd, likely reflecting the geology of the source ore deposit. Asmore »« less
https://doi.org/10.1016/j.talanta.2022.124088
Fractionation of Oxygen Isotopes in Uranium Oxides during Peroxide Precipitation and Dry Air Calcination

Journal Article Klosterman, Michael R. ; Oerter, Erik J. ; Chakraborty, Suvankar ; ... - ACS Earth and Space Chemistry

The interaction between uranium and oxygen-containing substrates is nearly ubiquitous within the nuclear fuel cycle. Given the well-known and predictable oxygen stable isotope compositions of atmospheric oxygen and meteoric waters around the world, the use of these isotopes as a potential geolocation or processing signature of uranium compounds has been of interest within the nuclear safeguards community. This study focuses on measuring the oxygen-stable isotope composition of synthetically produced uranium oxides to determine the mechanism and extent of fractionation during materials processing relevant to the nuclear fuel cycle. Here, metastudtite [UO₂O₂(H₂O)₂] samples were first produced using water and hydrogen peroxidemore »« less
https://doi.org/10.1021/acsearthspacechem.1c00112

Full Text Available
Compilation of LLNL CUP-2 Data

Technical Report Eppich, G. ; Kips, R. ; Lindvall, R.

The CUP-2 uranium ore concentrate (UOC) standard reference material, a powder, was produced at the Blind River uranium refinery of Eldorado Resources Ltd. in Canada in 1986. This material was produced as part of a joint effort by the Canadian Certified Reference Materials Project and the Canadian Uranium Producers Metallurgical Committee to develop a certified reference material for uranium concentration and the concentration of several impurity constituents. This standard was developed to satisfy the requirements of the UOC mining and milling industry, and was characterized with this purpose in mind. To produce CUP-2, approximately 25 kg of UOC derived frommore »« less
https://doi.org/10.2172/1325861

Full Text Available

Similar Records