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

Abstract

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 themore » 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.« less

Authors:
 [1]; ORCiD logo [2];  [2];  [2];  [1]
  1. Univ. of Munster (Germany); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); German Research Foundation (DFG)
OSTI Identifier:
1668482
Alternate Identifier(s):
OSTI ID: 1810950
Report Number(s):
LLNL-JRNL-811552
Journal ID: ISSN 0039-9140; 1018406
Grant/Contract Number:  
AC52-07NA27344; 440227108
Resource Type:
Accepted Manuscript
Journal Name:
Talanta
Additional Journal Information:
Journal Volume: 221; Journal ID: ISSN 0039-9140
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; Nuclear forensics; origin assessment; samarium isotopes; uranium ore concentrate; thermal neutron capture

Citation Formats

Shollenberger, Quinn R., Borg, Lars E., Ramon, Erick C., Sharp, Michael A., and Brennecka, Gregory A.. Samarium isotope compositions of uranium ore concentrates: A novel nuclear forensic signature. United States: N. p., 2020. Web. https://doi.org/10.1016/j.talanta.2020.121431.
Shollenberger, Quinn R., Borg, Lars E., Ramon, Erick C., Sharp, Michael A., & Brennecka, Gregory A.. Samarium isotope compositions of uranium ore concentrates: A novel nuclear forensic signature. United States. https://doi.org/10.1016/j.talanta.2020.121431
Shollenberger, Quinn R., Borg, Lars E., Ramon, Erick C., Sharp, Michael A., and Brennecka, Gregory A.. Fri . "Samarium isotope compositions of uranium ore concentrates: A novel nuclear forensic signature". United States. https://doi.org/10.1016/j.talanta.2020.121431. https://www.osti.gov/servlets/purl/1668482.
@article{osti_1668482,
title = {Samarium isotope compositions of uranium ore concentrates: A novel nuclear forensic signature},
author = {Shollenberger, Quinn R. and Borg, Lars E. and Ramon, Erick C. and Sharp, Michael A. and Brennecka, Gregory A.},
abstractNote = {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.},
doi = {10.1016/j.talanta.2020.121431},
journal = {Talanta},
number = ,
volume = 221,
place = {United States},
year = {2020},
month = {7}
}

Works referenced in this record:

The state of nuclear forensics
journal, January 2013

  • Kristo, Michael J.; Tumey, Scott J.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 294
  • DOI: 10.1016/j.nimb.2012.07.047

Nuclear Forensic Science: Analysis of Nuclear Material Out of Regulatory Control
journal, June 2016


Investigation of the sample characteristics needed for the determination of the origin of uranium-bearing materials
journal, June 2008

  • Švedkauskaitė-LeGore, J.; Rasmussen, G.; Abousahl, S.
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 278, Issue 1
  • DOI: 10.1007/s10967-007-7215-y

Application of Lead and Strontium Isotope Ratio Measurements for the Origin Assessment of Uranium Ore Concentrates
journal, October 2009

  • Varga, Zsolt; Wallenius, Maria; Mayer, Klaus
  • Analytical Chemistry, Vol. 81, Issue 20
  • DOI: 10.1021/ac901100e

Identification of uranium signatures relevant for nuclear safeguards and forensics
journal, April 2017

  • Varga, Zsolt; Krajkó, Judit; Peńkin, Maxim
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 312, Issue 3
  • DOI: 10.1007/s10967-017-5247-5

Natural variations in uranium isotope ratios of uranium ore concentrates: Understanding the 238U/235U fractionation mechanism
journal, March 2010

  • Brennecka, Gregory A.; Borg, Lars E.; Hutcheon, Ian D.
  • Earth and Planetary Science Letters, Vol. 291, Issue 1-4
  • DOI: 10.1016/j.epsl.2010.01.023

Investigation of the 236 U/ 238 U isotope abundance ratio in uranium ores and yellow cake samples
journal, March 2011


Attribution of uranium ore concentrates using elemental and anionic data
journal, August 2012


Measurement of the sulphur isotope ratio (34S/32S) in uranium ore concentrates (yellow cakes) for origin assessment
journal, January 2013

  • Han, Sun-Ho; Varga, Zsolt; Krajkó, Judit
  • Journal of Analytical Atomic Spectrometry, Vol. 28, Issue 12
  • DOI: 10.1039/c3ja50231g

Application of neodymium isotope ratio measurements for the origin assessment of uranium ore concentrates
journal, November 2014


Molybdenum isotope compositions of uranium ore concentrates by double spike MC-ICP-MS
journal, April 2019


Trace element and U isotope analysis of uraninite and ore concentrate: Applications for nuclear forensic investigations
journal, September 2017


In-situ production of natural 236U in groundwaters and ores in high-grade uranium deposits
journal, September 2015


The first detection of naturally-occurring 236U with accelerator mass spectrometry
journal, June 1994

  • 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
  • DOI: 10.1016/0168-583X(94)96014-3

Nucleogenic 36Cl, 236U and 239Pu in uranium ores
journal, August 2008

  • 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
  • DOI: 10.1016/j.nimb.2008.06.009

Isotopic “fingerprints” for natural uranium ore samples
journal, October 1999


Neutron capture effects on Sm and Gd isotopes in uraninites
journal, March 2001


Uranium and Sm isotope studies of the supergiant Olympic Dam Cu–Au–U–Ag deposit, South Australia
journal, May 2016


Neutron capture on149Sm in lunar samples
journal, December 1971


High fluences of neutrons determined from Sm and Gd isotopic compositions in aubrites
journal, November 1999

  • Hidaka, Hiroshi; Ebihara, Mitsuru; Yoneda, Shigekazu
  • Earth and Planetary Science Letters, Vol. 173, Issue 1-2
  • DOI: 10.1016/S0012-821X(99)00221-6

The Witwatersrand Basin, South Africa: Geological framework and mineralization processes
journal, December 1995


Genesis of Multifarious Uranium Mineralization in the Beaverlodge Area, Northern Saskatchewan, Canada
journal, November 2014


Zircon ages and Nd isotopic and chemical compositions of orthogneisses from the Black Forest, Germany: evidence for a Cambrian magmatic arc
journal, March 2000

  • Chen, F.; Hegner, E.; Todt, W.
  • International Journal of Earth Sciences, Vol. 88, Issue 4
  • DOI: 10.1007/s005310050306

Ages of some uranium and thorium minerals from East and Central Africa
journal, March 1961

  • Darnley, A. G.; Horne, J. E. T.; Smith, G. H.
  • Mineralogical Magazine and Journal of the Mineralogical Society, Vol. 32, Issue 252
  • DOI: 10.1180/minmag.1961.032.252.05

Trace element mobility in mine waters from granitic pegmatite U–Th–REE deposits, Bancroft area, Ontario
journal, April 2016


Geochronology of Precambrian granites and associated U-Ti-Th mineralization, northern Olary province, South Australia
journal, June 1984

  • Ludwig, K. R.; Cooper, J. A.
  • Contributions to Mineralogy and Petrology, Vol. 86, Issue 3
  • DOI: 10.1007/BF00373676

Origin assessment of uranium ore concentrates based on their rare-earth elemental impurity pattern
journal, January 2010

  • Varga, Zsolt; Wallenius, Maria; Mayer, Klaus
  • Radiochimica Acta, Vol. 98, Issue 12
  • DOI: 10.1524/ract.2010.1777

Uranium-Lead Ages of the Uranium Deposits of the Gas Hills and Shirley Basin, Wyoming
journal, July 1974


U-Pb geochronological constraints on the genesis of the Olympic Dam Cu-U-Au-Ag deposit, South Australia
journal, August 1995


Supergene processes and uranium ore formation in the Ronneburg ore field, Germany
journal, April 2012


Plant availability of uranium in contaminated soil from Crucea Mine (Romania)
journal, September 2003


The Schwartzwalder uranium deposit; II, Age of uranium mineralization and lead isotope constraints on genesis
journal, November 1985


Geochronology of Uraninite Revisited
journal, February 2020