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

Hunter B. Andrews, C. Derrick Quarles, Veronica C. Bradley, Tyler L. Spano, Joseph A. Petrus, Bence Paul, N. Alex Zirakparvar, Daniel R. Dunlap, Cole R. Hexel, Benjamin T. Manard

Research output: Contribution to journalArticlepeer-review

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Abstract

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. 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).

Original languageEnglish
Article number109605
JournalMicrochemical Journal
Volume196
DOIs
StatePublished - Jan 2024

Funding

This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (https://energy.gov/downloads/doe-public-access-plan). This work was supported by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy under contract DE-AC-05-000R22725. The authors would like to acknowledge Mark Boris (ORNL) for the assistance with optical images presented within this manuscript and Jacquelyn DeMink for the assistance with graphics.

FundersFunder number
Mark Boris
U.S. Department of EnergyDE-AC-05-000R22725
Oak Ridge National Laboratory

    Keywords

    • Elemental imaging
    • Finchite
    • ICP-MS
    • Isotopic ratios
    • LIBS
    • Laser-ablation
    • Uranium

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