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Direct Uranium Isotopic Analysis of Swipe Surfaces by Microextraction-ICP-MS
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    Direct Uranium Isotopic Analysis of Swipe Surfaces by Microextraction-ICP-MS
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    • Benjamin T. Manard*
      Benjamin T. Manard
      Oak Ridge National Laboratory, Chemical Sciences Division, 1 Bethel Valley Rd, Oak Ridge, Tennessee 37830, United States
      *Email: [email protected]
    • Kayron T. Rogers
      Kayron T. Rogers
      Oak Ridge National Laboratory, Chemical Sciences Division, 1 Bethel Valley Rd, Oak Ridge, Tennessee 37830, United States
    • Brian W. Ticknor
      Brian W. Ticknor
      Oak Ridge National Laboratory, Chemical Sciences Division, 1 Bethel Valley Rd, Oak Ridge, Tennessee 37830, United States
    • Shalina C. Metzger
      Shalina C. Metzger
      Oak Ridge National Laboratory, Chemical Sciences Division, 1 Bethel Valley Rd, Oak Ridge, Tennessee 37830, United States
    • N. Alex Zirakparvar
      N. Alex Zirakparvar
      Oak Ridge National Laboratory, Chemical Sciences Division, 1 Bethel Valley Rd, Oak Ridge, Tennessee 37830, United States
    • Benjamin D. Roach
      Benjamin D. Roach
      Oak Ridge National Laboratory, Chemical Sciences Division, 1 Bethel Valley Rd, Oak Ridge, Tennessee 37830, United States
    • Debra A. Bostick
      Debra A. Bostick
      Oak Ridge National Laboratory, Chemical Sciences Division, 1 Bethel Valley Rd, Oak Ridge, Tennessee 37830, United States
    • Cole R. Hexel
      Cole R. Hexel
      Oak Ridge National Laboratory, Chemical Sciences Division, 1 Bethel Valley Rd, Oak Ridge, Tennessee 37830, United States
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    Analytical Chemistry

    Cite this: Anal. Chem. 2021, 93, 32, 11133–11139
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    https://doi.org/10.1021/acs.analchem.1c01569
    Published July 8, 2021
    Copyright © 2021 American Chemical Society

    Abstract

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    The ability to directly measure uranium isotope ratios on environmental swipes has been achieved through a solution-based microextraction process and represents a significant advancement toward the development of a rapid method to analyze international nuclear safeguard samples. Here, a microextraction probe is lowered and sealed onto the swipe surface, and analytes within the sampling site (∼8 mm2) are dissolved and extracted into a flowing solvent of 2% nitric acid (HNO3). The mobilized species are subsequently directed into an inductively coupled plasma-mass spectrometer (ICP-MS) for accurate and precise isotope ratio determination. This work highlights the novelty of the sampling mechanism, particularly with the direct coupling of the microextraction probe to the ICP-MS and measurement of uranium isotope ratios. The preliminary method detection limit for the microextraction-ICP-MS method, utilizing a quadrupole-based MS, was determined to be ∼50 pg of 238U. Additionally, precise and accurate isotope ratio measurements were achieved on uranium reference materials for both the major (235U/238U) and minor (234U/238U and 236U/238U) ratios. While the present work is focused on directly measuring uranium isotopic systems on swipe surfaces for nuclear safeguards and verification applications, the benefits would extend across many applications in which direct solid sampling is sought for elemental and isotopic analysis.

    Copyright © 2021 American Chemical Society

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    Cited By

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    This article is cited by 11 publications.

    1. Jordan S. Stanberry, Hunter B. Andrews, Cyril V. Thompson, Brian W. Ticknor, Benjamin T. Manard. Microextraction-Single Particle-Inductively Coupled Plasma-Mass Spectrometry for the Direct Analysis of Nanoparticles on Surfaces. Analytical Chemistry 2025, Article ASAP.
    2. Veronica C. Bradley, Brian W. Ticknor, Daniel R. Dunlap, N. Alex Zirakparvar, Shalina C. Metzger, Cole R. Hexel, Benjamin T. Manard. Microextraction–TQ–ICP–MS for the Direct Analysis of U and Pu from Cotton Swipes. Analytical Chemistry 2023, 95 (43) , 15867-15874. https://doi.org/10.1021/acs.analchem.3c01022
    3. N. Alex Zirakparvar, Benjamin T. Manard, Daniel R. Dunlap, Brian Ticknor, Matt Darnell, Shalina C. Metzger, Cole R. Hexel. Exploration of metallic interferences pertinent to nuclear safeguards related uranium isotope ratio measurement on the Neoma MC-ICP-MS platform without the MS/MS option. International Journal of Mass Spectrometry 2024, 503 , 117278. https://doi.org/10.1016/j.ijms.2024.117278
    4. Sean R. Scott, Kirby P. Hobbs, Amanda D. French, Isaac J. Arnquist, Sonia Alcantar Anguiano, Daniel L. Sullivan, Staci M. Herman. Uranium isotopic analysis in unpurified solutions by ICP-MS. Journal of Analytical Atomic Spectrometry 2024, 39 (8) , 2106-2115. https://doi.org/10.1039/D4JA00130C
    5. Veronica C. Bradley, Jacob Burleson, Hunter B. Andrews, Cyril V. Thompson, Tyler L. Spano, Daniel R. Dunlap, N. Alex Zirakparvar, Brian W. Ticknor, Cole R. Hexel, Benjamin T. Manard. Mapping of uranium particles on J-type swipes with microextraction-ICP-MS. The Analyst 2024, 149 (8) , 2244-2251. https://doi.org/10.1039/D3AN02101G
    6. Joseph V. Goodwin, Benjamin T. Manard, Brian W. Ticknor, Paula Cable-Dunlap, R. Kenneth Marcus. Investigation of potential polyatomic interferences on uranium isotope ratio measurements for the LS-APGD-Orbitrap MS system. Microchemical Journal 2024, 196 , 109645. https://doi.org/10.1016/j.microc.2023.109645
    7. Cameron J. Stouffer, R. Kenneth Marcus. Direct, multielement determinations from cotton swipes via plate express microextraction coupled to an inductively coupled plasma mass spectrometer (μEx-ICP-MS). Journal of Analytical Atomic Spectrometry 2023, 38 (10) , 1943-1951. https://doi.org/10.1039/D3JA00248A
    8. Joseph V. Goodwin, Benjamin T. Manard, R. Kenneth Marcus, Brian W. Ticknor, Paula Cable-Dunlap. Investigation of Potential Polyatomic Interferences on Uranium Isotope Ratio Measurements for the Ls-Apgd-Orbitrap Ms System. 2023https://doi.org/10.2139/ssrn.4617608
    9. Veronica C. Bradley, Tyler L. Spano, Cyril V. Thompson, Brian W. Ticknor, Daniel R. Dunlap, Shalina C. Metzger, Cole R. Hexel, Benjamin T. Manard. Analysis of solid uranium particulates on cotton swipes with an automated microextraction-ICP-MS system. Analytical Methods 2022, 14 (44) , 4466-4473. https://doi.org/10.1039/D2AY01394K
    10. Veronica C. Bradley, Tyler L. Spano, Shalina C. Metzger, Brian W. Ticknor, Daniel R. Dunlap, N. Alex Zirakparvar, Benjamin D. Roach, Cole R. Hexel, Benjamin T. Manard. Direct isotopic analysis of solid uranium particulates on cotton swipes by microextraction-ICP-MS. Analytica Chimica Acta 2022, 1209 , 339836. https://doi.org/10.1016/j.aca.2022.339836
    11. Shuming Peng, Taiping Peng, Guangai Sun. Progress on nuclear analysis techniques. Nuclear Analysis 2022, 1 (1) , 100007. https://doi.org/10.1016/j.nucana.2022.100007
    12. Benjamin T. Manard, Shalina C. Metzger, Kayron T. Rogers, Brian W. Ticknor, N. Alex Zirakparvar, Benjamin D. Roach, Debra A. Bostick, Cole R. Hexel. Direct analysis of cotton swipes for plutonium isotope determination by microextraction-ICP-MS. Journal of Analytical Atomic Spectrometry 2021, 36 (10) , 2202-2209. https://doi.org/10.1039/D1JA00255D

    Analytical Chemistry

    Cite this: Anal. Chem. 2021, 93, 32, 11133–11139
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.analchem.1c01569
    Published July 8, 2021
    Copyright © 2021 American Chemical Society

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