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

Shollenberger, Quinn R.; Borg, Lars E.; Ramon, Erick C.; Sharp, Michael A.; Brennecka, Gregory A.

doi:10.1016/j.talanta.2020.121431

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

Journal Article · Fri Jul 31 00:00:00 EDT 2020 · Talanta

DOI:https://doi.org/10.1016/j.talanta.2020.121431· OSTI ID:1668482

Shollenberger, Quinn R. ^[1]; ^[2]; Ramon, Erick C. ^[2]; Sharp, Michael A. ^[2]; Brennecka, Gregory A. ^[1]

Univ. of Munster (Germany); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

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 a new method to separate samarium (Sm) from a U-rich sample matrix and report the first Sm isotope compositions of 32 UOCs derived from a variety of worldwide uranium mines. Relative to terrestrial standards, approximately half the UOCs have resolved and anticorrelated ¹⁴⁹Sm-¹⁵⁰Sm isotope compositions, consistent with the capture of thermal neutrons by ¹⁴⁹Sm in the ore body. The UOCs with anomalous Sm isotope compositions tend to derive from older (~>1.5Ga) and higher-grade ore bodies, although other factors, such as the presence of neutron moderators like water, also play a role. Nonetheless, the Sm isotope compositions of UOCs directly reflects the neutron fluence over the history of the original ore body and can be used to discern different geologic conditions associated with that ore body. Overall, this work demonstrates the potential use of Sm isotopes as a novel nuclear forensics signature for origin assessment of UOCs.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: German Research Foundation (DFG); USDOE; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1668482

Alternate ID(s):: OSTI ID: 1810950

Report Number(s):: LLNL-JRNL--811552; 1018406

Journal Information:: Talanta, Journal Name: Talanta Vol. 221; ISSN 0039-9140

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (38)

Geochronology of Precambrian granites and associated U-Ti-Th mineralization, northern Olary province, South Australia Ludwig, K. R.; Cooper, J. A. Contributions to Mineralogy and Petrology, Vol. 86, Issue 3 https://doi.org/10.1007/BF00373676	journal	June 1984
Zircon ages and Nd isotopic and chemical compositions of orthogneisses from the Black Forest, Germany: evidence for a Cambrian magmatic arc Chen, F.; Hegner, E.; Todt, W. International Journal of Earth Sciences, Vol. 88, Issue 4 https://doi.org/10.1007/s005310050306	journal	March 2000
Investigation of the sample characteristics needed for the determination of the origin of uranium-bearing materials Švedkauskaitė-LeGore, J.; Rasmussen, G.; Abousahl, S. Journal of Radioanalytical and Nuclear Chemistry, Vol. 278, Issue 1 https://doi.org/10.1007/s10967-007-7215-y	journal	June 2008
Identification of uranium signatures relevant for nuclear safeguards and forensics Varga, Zsolt; Krajkó, Judit; Peńkin, Maxim Journal of Radioanalytical and Nuclear Chemistry, Vol. 312, Issue 3 https://doi.org/10.1007/s10967-017-5247-5	journal	April 2017
A search for fossil nuclear reactors in the Alligator River Uranium Field, Australia: Constraints from Sm, Gd and Nd isotopic studies Maas, R.; McCulloch, M. T. Chemical Geology, Vol. 88, Issue 3-4 https://doi.org/10.1016/0009-2541(90)90095-O	journal	November 1990
Neutron capture on149Sm in lunar samples Russ, G. P.; Burnett, D. S.; Lingenfelter, R. E. Earth and Planetary Science Letters, Vol. 13, Issue 1 https://doi.org/10.1016/0012-821X(71)90104-X	journal	December 1971
The first detection of naturally-occurring 236U with accelerator mass spectrometry Zhao, X-L.; Nadeau, M-J.; Kilius, L. R. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 92, Issue 1-4 https://doi.org/10.1016/0168-583X(94)96014-3	journal	June 1994
The Witwatersrand Basin, South Africa: Geological framework and mineralization processes Robb, Laurence J.; Meyer, F. Michael Ore Geology Reviews, Vol. 10, Issue 2 https://doi.org/10.1016/0169-1368(95)00011-9	journal	December 1995
High fluences of neutrons determined from Sm and Gd isotopic compositions in aubrites Hidaka, Hiroshi; Ebihara, Mitsuru; Yoneda, Shigekazu Earth and Planetary Science Letters, Vol. 173, Issue 1-2 https://doi.org/10.1016/S0012-821X(99)00221-6	journal	November 1999
Neutron capture effects on Sm and Gd isotopes in uraninites Hidaka, Hiroshi; Gauthier-Lafaye, Francois Geochimica et Cosmochimica Acta, Vol. 65, Issue 6 https://doi.org/10.1016/S0016-7037(00)00567-6	journal	March 2001
Natural nuclear fission reactors: time constraints for occurrence, and their relation to uranium and manganese deposits and to the evolution of the atmosphere Gauthier-Lafaye, François; Weber, Francis Precambrian Research, Vol. 120, Issue 1-2 https://doi.org/10.1016/S0301-9268(02)00163-8	journal	January 2003
Isotopic “fingerprints” for natural uranium ore samples Richter, S.; Alonso, A.; De Bolle, W. International Journal of Mass Spectrometry, Vol. 193, Issue 1 https://doi.org/10.1016/S1387-3806(99)00102-5	journal	October 1999
Attribution of uranium ore concentrates using elemental and anionic data Keegan, Elizabeth; Wallenius, Maria; Mayer, Klaus Applied Geochemistry, Vol. 27, Issue 8 https://doi.org/10.1016/j.apgeochem.2012.05.009	journal	August 2012
Trace element mobility in mine waters from granitic pegmatite U–Th–REE deposits, Bancroft area, Ontario Desbarats, A. J.; Percival, J. B.; Venance, K. E. Applied Geochemistry, Vol. 67 https://doi.org/10.1016/j.apgeochem.2016.02.010	journal	April 2016
Trace element and U isotope analysis of uraninite and ore concentrate: Applications for nuclear forensic investigations Spano, Tyler L.; Simonetti, Antonio; Balboni, Enrica Applied Geochemistry, Vol. 84 https://doi.org/10.1016/j.apgeochem.2017.07.003	journal	September 2017
Molybdenum isotope compositions of uranium ore concentrates by double spike MC-ICP-MS Rolison, John M.; Druce, Matthew; Shollenberger, Quinn R. Applied Geochemistry, Vol. 103 https://doi.org/10.1016/j.apgeochem.2019.03.001	journal	April 2019
In-situ production of natural 236U in groundwaters and ores in high-grade uranium deposits Murphy, Melissa J.; Froehlich, Michaela B.; Fifield, L. Keith Chemical Geology, Vol. 410 https://doi.org/10.1016/j.chemgeo.2015.06.024	journal	September 2015
Natural variations in uranium isotope ratios of uranium ore concentrates: Understanding the 238U/235U fractionation mechanism Brennecka, Gregory A.; Borg, Lars E.; Hutcheon, Ian D. Earth and Planetary Science Letters, Vol. 291, Issue 1-4 https://doi.org/10.1016/j.epsl.2010.01.023	journal	March 2010
Uranium and Sm isotope studies of the supergiant Olympic Dam Cu–Au–U–Ag deposit, South Australia Kirchenbaur, Maria; Maas, Roland; Ehrig, Kathy Geochimica et Cosmochimica Acta, Vol. 180 https://doi.org/10.1016/j.gca.2016.01.035	journal	May 2016
Optimization of the in-situ U–Pb age dating method via LA-Quadrupole-ICP-MS with applications to the timing of U–Zr–Mo mineralization in the Poços de Caldas Alkaline Complex, SE Brazil Takenaka, Lynthener Bianca; Lana, Cristiano; Scholz, Ricardo Journal of South American Earth Sciences, Vol. 62 https://doi.org/10.1016/j.jsames.2015.04.007	journal	October 2015
Nucleogenic 36Cl, 236U and 239Pu in uranium ores Wilcken, K. M.; Fifield, L. K.; Barrows, T. T. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 266, Issue 16 https://doi.org/10.1016/j.nimb.2008.06.009	journal	August 2008
The state of nuclear forensics Kristo, Michael J.; Tumey, Scott J. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 294 https://doi.org/10.1016/j.nimb.2012.07.047	journal	January 2013
Application of neodymium isotope ratio measurements for the origin assessment of uranium ore concentrates Krajkó, Judit; Varga, Zsolt; Yalcintas, Ezgi Talanta, Vol. 129 https://doi.org/10.1016/j.talanta.2014.06.022	journal	November 2014
Application of Lead and Strontium Isotope Ratio Measurements for the Origin Assessment of Uranium Ore Concentrates Varga, Zsolt; Wallenius, Maria; Mayer, Klaus Analytical Chemistry, Vol. 81, Issue 20 https://doi.org/10.1021/ac901100e	journal	October 2009
Measurement of the sulphur isotope ratio (34S/32S) in uranium ore concentrates (yellow cakes) for origin assessment Han, Sun-Ho; Varga, Zsolt; Krajkó, Judit Journal of Analytical Atomic Spectrometry, Vol. 28, Issue 12 https://doi.org/10.1039/c3ja50231g	journal	January 2013
Origin of uranium deposits revealed by their rare earth element signature: Origin of U deposits revealed by the rare earth elements Mercadier, Julien; Cuney, Michel; Lach, Philippe Terra Nova, Vol. 23, Issue 4 https://doi.org/10.1111/j.1365-3121.2011.01008.x	journal	May 2011
U-Pb ages of ferberite, chalcedony, agate, 'U-mica' and pitchblende: constraints on the mineralization history of the Schwarzwald ore district [U-Pb ages of ferberite, chalcedony, agate, 'U-mica' and pitchblende: constraints on the mineralization history of the Schwarzwald ore district] Pfaff, Katharina; Romer, Rolf L.; Markl, Gregor European Journal of Mineralogy, Vol. 21, Issue 4 https://doi.org/10.1127/0935-1221/2009/0021-1944	journal	August 2009
Supergene processes and uranium ore formation in the Ronneburg ore field, Germany Bolonin, A. V.; Gradovsky, I. F. Geology of Ore Deposits, Vol. 54, Issue 2 https://doi.org/10.1134/S1075701512020031	journal	April 2012
Nuclear Forensic Science: Analysis of Nuclear Material Out of Regulatory Control Kristo, Michael J.; Gaffney, Amy M.; Marks, Naomi Annual Review of Earth and Planetary Sciences, Vol. 44, Issue 1 https://doi.org/10.1146/annurev-earth-060115-012309	journal	June 2016
Ages of some uranium and thorium minerals from East and Central Africa Darnley, A. G.; Horne, J. E. T.; Smith, G. H. Mineralogical Magazine and Journal of the Mineralogical Society, Vol. 32, Issue 252 https://doi.org/10.1180/minmag.1961.032.252.05	journal	March 1961
Plant availability of uranium in contaminated soil from Crucea Mine (Romania) Petrescu, L.; Bilal, E. Environmental Geosciences, Vol. 10, Issue 3 https://doi.org/10.1306/eg100302001	journal	September 2003
Origin assessment of uranium ore concentrates based on their rare-earth elemental impurity pattern Varga, Zsolt; Wallenius, Maria; Mayer, Klaus Radiochimica Acta, Vol. 98, Issue 12 https://doi.org/10.1524/ract.2010.1777	journal	January 2010
Investigation of the ²³⁶ U/ ²³⁸ U isotope abundance ratio in uranium ores and yellow cake samples Srncik, M.; Mayer, K.; Hrnecek, Erich Radiochimica Acta, Vol. 99, Issue 6 https://doi.org/10.1524/ract.2011.1840	journal	March 2011
Genesis of Multifarious Uranium Mineralization in the Beaverlodge Area, Northern Saskatchewan, Canada Dieng, S.; Kyser, K.; Godin, L. Economic Geology, Vol. 110, Issue 1 https://doi.org/10.2113/econgeo.110.1.209	journal	November 2014
Uranium-Lead Ages of the Uranium Deposits of the Gas Hills and Shirley Basin, Wyoming Dooley, J. R.; Harshman, E. N.; Rosholt, J. N. Economic Geology, Vol. 69, Issue 4 https://doi.org/10.2113/gsecongeo.69.4.527	journal	July 1974
The Schwartzwalder uranium deposit; II, Age of uranium mineralization and lead isotope constraints on genesis Ludwig, K. R.; Wallace, Alan R.; Simmons, K. R. Economic Geology, Vol. 80, Issue 7 https://doi.org/10.2113/gsecongeo.80.7.1858	journal	November 1985
U-Pb geochronological constraints on the genesis of the Olympic Dam Cu-U-Au-Ag deposit, South Australia Johnson, James P.; Cross, Ken C. Economic Geology, Vol. 90, Issue 5 https://doi.org/10.2113/gsecongeo.90.5.1046	journal	August 1995
Geochronology of Uraninite Revisited Corcoran, Loretta; Simonetti, Antonio Minerals, Vol. 10, Issue 3 https://doi.org/10.3390/min10030205	journal	February 2020

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58 GEOSCIENCES
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samarium isotopes
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Samarium isotope compositions of uranium ore concentrates: A novel nuclear forensic signature

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