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Title: Advancing Elemental and Isotopic Analysis of Uranium Mineral Inclusions: Rapid Screening via Laser-Induced Breakdown Spectroscopy and High-Resolution Laser Ablation-ICP-MS Mapping

Journal Article · · Microchemical Journal
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
  2. Elemental Scientific Inc., Omaha, NE (United States)
  3. Elemental Scientific Lasers, Bozeman, MT (United States)
  4. Elemental Scientific Lasers, Bozeman, MT (United States); Univ. of Melbourne, Parkville, VIC (Australia)
+ Show Author Affiliations

The work presented herein employs two laser-based analytical techniques (laser-induced breakdown spectroscopy (LIBS) and laser ablation – inductively coupled plasma – mass spectrometry (LA-ICP-MS)) to spatially determine the elemental and isotopic composition of uranium bearing minerals. Uniquely, this work leverages the high-speed applicability of LIBS to “screen” the sample(s) for their elemental constituents. After determining the location of the uranium inclusions (via LIBS), high-resolution LA-ICP-MS was employed to further characterize the inclusions. The high-resolution (sub-µm) capabilities of LA-ICP-MS were able to extract important information from the uranium minerals including discerning its chemical form (e.g., finchite from carnotite, Sr- and K-bearing uranyl vanadates, respectively) as well as their 235U/238U isotopic composition. This approach, LIBS followed by LA-ICP-MS, significantly reduces the analysis time (~95 %) in comparison to employing a LA-ICP-MS only approach. Furthermore, this work presented a novel approach to analyzing inclusions via a particle/inclusion analysis tool which is commercially available within the iolite 4 software. This tool allowed for a more accurate characterization of the isotopic distribution of the inclusions, as well as allowing for rapid sizing of the inclusions. Finally, this analytical approach could readily be applied to other sample types in which the target species (e.g., µm-sized inclusions) are embedded in complex matrices (e.g., cm-sized samples).

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Laboratory Directed Research and Development (LDRD) Program
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
2229224
Alternate ID(s):
OSTI ID: 2369124
Journal Information:
Microchemical Journal, Journal Name: Microchemical Journal Journal Issue: 1 Vol. 196; ISSN 0026-265X
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (23)

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Application of laser ablation inductively coupled plasma mass spectrometry for the isotopic analysis of single uranium particles journal September 2008
Chenowethite, Mg(H2O)6[(UO2)2(SO4)2(OH)2]·5H2O, a New Mineral with Uranyl-Sulfate Sheets from Red Canyon, Utah, USA journal December 2022
Capabilities of laser ablation – ICP-TOF-MS coupling for isotopic analysis of individual uranium micrometric particles journal January 2018
A Revised and Expanded Structure Hierarchy of Natural and Synthetic Hexavalent Uranium Compounds journal January 2016
Analytical performance of a high-repetition rate laser head (500 Hz) for HR LA-ICP-QMS imaging journal January 2020
Performance of laser ablation: quadrupole-based ICP-MS coupling for the analysis of single micrometric uranium particles journal September 2012
Assessment of uranium inhomogeneity and isotope imaging for nuclear forensics journal September 2020
Finchite, Sr(UO2)2(V2O8)·5H2O, a new uranyl sorovanadate with the francevillite anion topology journal February 2023
Calcrete uranium deposits in the Southern High Plains, USA journal June 2019
Laser-Induced Breakdown Spectroscopy Imaging for Material and Biomedical Applications: Recent Advances and Future Perspectives journal January 2023
Direct uranium isotope ratio analysis of single micrometer-sized glass particles journal November 2012
Quantitative elemental mapping of chondritic meteorites using laser ablation-inductively coupled plasma-time of flight-mass spectrometry (LA-ICP-TOF-MS) journal January 2023
Dual imaging of uranium ore by Laser Ablation Inductively Coupled Plasma Mass Spectrometry and Laser Induced Breakdown Spectroscopy journal December 2021
Recent developments in the design of rapid response cells for laser ablation-inductively coupled plasma-mass spectrometry and their impact on bioimaging applications journal January 2016
Insights into the selection of 2D LA-ICP-MS (multi)elemental mapping conditions journal January 2019
Oxidation-hydration weathering of uraninite: the current state-of-knowledge journal April 2014
U6+ Minerals and Inorganic Compounds: Insights into an Expanded Structural Hierarchy of Crystal Structures journal December 2005
Laser ablation – inductively couple plasma – mass spectrometry/laser induced break down spectroscopy: a tandem technique for uranium particle characterization journal January 2017
Determination of fluorine distribution in shark teeth by laser-induced breakdown spectroscopy journal July 2022
Methodology and applications of elemental mapping by laser induced breakdown spectroscopy journal February 2021
Review of the recent advances and applications of LIBS-based imaging journal January 2019
Sub-micrometer Nanosecond LA-ICP-MS Imaging at Pixel Acquisition Rates above 250 Hz via a Low-Dispersion Setup journal March 2020

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
LIBS
laser-ablation
ICP-MS
elemental imaging
isotropic ratios
Finchite
Uranium