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Title: Rare-earth element fractionation in uranium ore and its U(VI) alteration minerals

Journal Article · · Applied Geochemistry
 [1];  [2];  [2];  [2];  [3]
  1. Univ. of Notre Dame, IN (United States). Dept. of Civil and Environmental Engineering and Earth Science; Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Glenn T. Seaborg Inst.
  2. Univ. of Notre Dame, IN (United States). Dept. of Civil and Environmental Engineering and Earth Science
  3. Univ. of Notre Dame, IN (United States). Dept. of Civil and Environmental Engineering and Earth Science, Dept. of Chemistry and Biochemistry

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 uranium alteration phases. The results for U(VI) alteration minerals of two samples indicate enrichment of the light REEs (LREEs) over the heavy REEs (HREEs). This differential mobilization is attributed to differences in the mineralogical composition of the U(VI) alteration. There is a lack of fractionation of the LREEs in the uraninite alteration rind that is composed of U(VI) minerals containing Ca2+ as the interlayer cation (uranophane and bequerelite); contrarily, U(VI) alteration minerals containing K+ and Pb2+ as interlayer cations (fourmarierite, dumontite) indicate fractionation (enrichment) of the LREEs. Our results have implications for nuclear forensic analyses since a comparison is reported between the REE abundances for the CUP-2 (processed uranium ore) certified reference material and previously determined values for uranium ore concentrate (UOC) produced from the same U deposit (Blind River/Elliott Lake, Canada). UOCs represent the most common form of interdicted nuclear material and consequently is material frequently targeted for forensic analysis. The comparison reveals similar chondrite normalized REE signatures but variable absolute abundances. Based on the results reported here, the latter may be attributed to the differing REE abundances between primary ore and associated alteration phases, and/or is related to varying fabrication processes adopted during production of UOC.

Research Organization:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC52-07NA27344
OSTI ID:
1416495
Alternate ID(s):
OSTI ID: 1549381
Report Number(s):
LLNL-JRNL-725124
Journal Information:
Applied Geochemistry, Vol. 87, Issue C; ISSN 0883-2927
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 16 works
Citation information provided by
Web of Science

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Cenozoic oxidation episodes in West Africa at the origin of the in situ supergene mineral redistribution of the primary uranium orebodies (Imouraren deposit, Tim Mersoï Basin, Northern Niger) journal December 2019
What’s that yellow powder? A nuclear forensic case study journal August 2018
Characterization of uraninite using a FIB–SEM approach and its implications for LA–ICP–MS analyses journal October 2018
Avoiding polyatomic interferences in measurements of lanthanides in uranium material for nuclear forensic purposes journal June 2019
Happy Jack Uraninite: A New Reference Material for High Spatial Resolution Analysis of U‐Rich Matrices journal September 2019
Multivariate Analysis Based on Geochemical, Isotopic, and Mineralogical Compositions of Uranium-Rich Samples journal September 2019