Round Robin Analysis of Uranium Isotopics on Cotton Swipes Measured Using Microextraction-Based Sampling Versus Conventional Bulk Analysis

Metzger, Shalina C.; Bradley, Veronica C.; Ticknor, Brian W.; Hexel, Cole R.; Adkisson, Melissa L.; Zirakparvar, N. Alex; Dunlap, Daniel R.; Marcus, R. Kenneth; Goodwin, Joseph V.; Andrews, Hunter B.; Manard, Benjamin T.

doi:10.1177/27551857251367770

Round Robin Analysis of Uranium Isotopics on Cotton Swipes Measured Using Microextraction-Based Sampling Versus Conventional Bulk Analysis

Journal Article · Wed Aug 20 00:00:00 EDT 2025 · Applied Spectroscopy Practica

DOI:https://doi.org/10.1177/27551857251367770· OSTI ID:2997047

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Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Clemson University, SC (United States)

A comparison of microextraction sampling methods to directly analyze uranium isotopics on cotton swipes was performed concurrently with traditional bulk-processing methods. For the microextraction sampling approach, two different detection platforms were evaluated, a quadrupole-based inductively coupled plasma mass spectrometer (ICP-MS) and the liquid sampling-atmospheric pressure glow discharge (LS-APGD) coupled to an Orbitrap mass spectrometer. Results presented from this innovative sampling approach (i.e., microextraction) are compared with a more traditional approach employed for analysis of cotton-based environmental swipes, namely bulk ashing/digestion, separation, and subsequent analysis by high-precision multi-collector ICP-MS. Overall, the microextraction approach proved to be a reliable and accurate means to determine isotopic ratios of uranium collected on cotton swipes. The ICP-MS-based detection had relative standard deviations of <0.65% for the major isotopic determinations, whereas the LS-APGD-Orbitrap method had relative standard deviations of <3%. The percent relative difference for the ²³⁵U/²³⁸U ratios, in comparison to the expected values, was <1% for ICP-MS and <4% for the microplasma-Orbitrap method. Additionally, the microextraction ICP-MS accurately (<2%) and precisely (<5%) determined the minor isotopic compositions (i.e., ²³⁴U/²³⁸U and ²³⁶U/²³⁸U).

View Accepted Manuscript (DOE)

Research Organization:: University of Florida, Gainesville, FL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Clemson University, SC (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation

Grant/Contract Number:: NA0004142; AC05-00OR22725

OSTI ID:: 2997047

Alternate ID(s):: OSTI ID: 3002506

Journal Information:: Applied Spectroscopy Practica, Journal Name: Applied Spectroscopy Practica Journal Issue: 3 Vol. 3; ISSN 2755-1857

Publisher:: SAGECopyright Statement

Country of Publication:: United States

Language:: English

References (25)

Preliminary investigation of an uncertainty budget for uranium isotope ratio analysis using a liquid sampling—atmospheric pressure glow discharge—orbitrap mass spectrometer system Goodwin, Joseph V.; Manard, Benjamin T.; Ticknor, Brian W. Journal of Radioanalytical and Nuclear Chemistry, Vol. 332, Issue 7 https://doi.org/10.1007/s10967-023-08901-9	journal	June 2023
Preliminary Figures of Merit for Isotope Ratio Measurements: The Liquid Sampling-Atmospheric Pressure Glow Discharge Microplasma Ionization Source Coupled to an Orbitrap Mass Analyzer Hoegg, Edward D.; Barinaga, Charles J.; Hager, George J. Journal of The American Society for Mass Spectrometry, Vol. 27, Issue 8 https://doi.org/10.1007/s13361-016-1402-4	journal	April 2016
Strengthening IAEA safeguards through environmental sampling and analysis Donohue, D. L. Journal of Alloys and Compounds, Vol. 271-273 https://doi.org/10.1016/S0925-8388(98)00015-2	journal	June 1998
Direct isotopic analysis of solid uranium particulates on cotton swipes by microextraction-ICP-MS Bradley, Veronica C.; Spano, Tyler L.; Metzger, Shalina C. Analytica Chimica Acta, Vol. 1209 https://doi.org/10.1016/j.aca.2022.339836	journal	May 2022
Implementation of Guide to the expression of Uncertainty in Measurement (GUM) to multi-collector TIMS uranium isotope ratio metrology Bürger, S.; Essex, R. M.; Mathew, K. J. International Journal of Mass Spectrometry, Vol. 294, Issue 2-3 https://doi.org/10.1016/j.ijms.2010.05.003	journal	July 2010
Roles of collisional dissociation modalities on spectral composition and isotope ratio measurement performance of the liquid sampling – atmospheric pressure glow discharge / orbitrap mass spectrometer coupling Williams, Tyler J.; Hoegg, Edward D.; Bills, Jacob R. International Journal of Mass Spectrometry, Vol. 464 https://doi.org/10.1016/j.ijms.2021.116572	journal	June 2021
Investigation of potential polyatomic interferences on uranium isotope ratio measurements for the LS-APGD-Orbitrap MS system Goodwin, Joseph V.; Manard, Benjamin T.; Ticknor, Brian W. Microchemical Journal, Vol. 196 https://doi.org/10.1016/j.microc.2023.109645	journal	January 2024
Optimization of uranium and plutonium separations using TEVA and UTEVA cartridges for MC-ICP-MS analysis of environmental swipe samples Metzger, Shalina C.; Rogers, Kayron T.; Bostick, Debra A. Talanta, Vol. 198 https://doi.org/10.1016/j.talanta.2019.02.034	journal	June 2019
Quantification of uranium, plutonium, neodymium and gadolinium for the characterization of spent nuclear fuel using isotope dilution HPIC-SF-ICP-MS Wanna, Nancy Nazem; Dobney, Andrew; Van Hoecke, Karen Talanta, Vol. 221 https://doi.org/10.1016/j.talanta.2020.121592	journal	January 2021
The need for speed – Burnup determination of spent nuclear fuel Roach, Benjamin D.; Rogers, Kayron T.; Zirakparvar, N. Alex Talanta Open, Vol. 6 https://doi.org/10.1016/j.talo.2022.100152	journal	December 2022
Rapid Determination of Uranium Isotopic Abundance from Cotton Swipes: Direct Extraction via a Planar Surface Reader and Coupling to a Microplasma Ionization Source Paing, Htoo W.; Manard, Benjamin T.; Ticknor, Brian W. Analytical Chemistry, Vol. 92, Issue 12 https://doi.org/10.1021/acs.analchem.0c01606	journal	June 2020
Direct Uranium Isotopic Analysis of Swipe Surfaces by Microextraction-ICP-MS Manard, Benjamin T.; Rogers, Kayron T.; Ticknor, Brian W. Analytical Chemistry, Vol. 93, Issue 32 https://doi.org/10.1021/acs.analchem.1c01569	journal	July 2021
Microextraction–TQ–ICP–MS for the Direct Analysis of U and Pu from Cotton Swipes Bradley, Veronica C.; Ticknor, Brian W.; Dunlap, Daniel R. Analytical Chemistry, Vol. 95, Issue 43 https://doi.org/10.1021/acs.analchem.3c01022	journal	October 2023
Microextraction-Single Particle-Inductively Coupled Plasma-Mass Spectrometry for the Direct Analysis of Nanoparticles on Surfaces Stanberry, Jordan S.; Andrews, Hunter B.; Thompson, Cyril V. Analytical Chemistry, Vol. 97, Issue 3 https://doi.org/10.1021/acs.analchem.4c04794	journal	January 2025
Automated Separation of Uranium and Plutonium from Environmental Swipe Samples for Multiple Collector Inductively Coupled Plasma Mass Spectrometry Metzger, Shalina C.; Ticknor, Brian W.; Rogers, Kayron T. Analytical Chemistry, Vol. 90, Issue 15 https://doi.org/10.1021/acs.analchem.8b02095	journal	June 2018
Improved Uranium Isotope Ratio Analysis in Liquid Sampling–Atmospheric Pressure Glow Discharge/Orbitrap FTMS Coupling through the Use of an External Data Acquisition System Bills, Jacob R.; Nagornov, Konstantin O.; Kozhinov, Anton N. Journal of the American Society for Mass Spectrometry, Vol. 32, Issue 5 https://doi.org/10.1021/jasms.1c00051	journal	April 2021
Rapid separation of uranium and plutonium by extraction chromatography for determination by thermal ionisation mass spectrometry Goodall, P.; Lythgoe, C. The Analyst, Vol. 124, Issue 3 https://doi.org/10.1039/A809219B	journal	January 1999
Mass spectrometric analysis for nuclear safeguards Boulyga, Sergei; Konegger-Kappel, Stefanie; Richter, Stephan Journal of Analytical Atomic Spectrometry, Vol. 30, Issue 7 https://doi.org/10.1039/C4JA00491D	journal	January 2015
Uranium isotope analysis by MC-ICP-MS in sub-ng sized samples Boulyga, Sergei F.; Koepf, Andreas; Konegger-Kappel, Stefanie Journal of Analytical Atomic Spectrometry, Vol. 31, Issue 11 https://doi.org/10.1039/C6JA00238B	journal	January 2016
A multi-electrode glow discharge ionization source for atomic and molecular mass spectrometry Hoegg, Edward D.; Williams, Tyler J.; Bills, Jacob R. Journal of Analytical Atomic Spectrometry, Vol. 35, Issue 9 https://doi.org/10.1039/D0JA00142B	journal	January 2020
Direct analysis of cotton swipes for plutonium isotope determination by microextraction-ICP-MS Manard, Benjamin T.; Metzger, Shalina C.; Rogers, Kayron T. Journal of Analytical Atomic Spectrometry, Vol. 36, Issue 10 https://doi.org/10.1039/D1JA00255D	journal	January 2021
Direct, multielement determinations from cotton swipes via plate express microextraction coupled to an inductively coupled plasma mass spectrometer (μEx-ICP-MS) Stouffer, Cameron J.; Marcus, R. Kenneth Journal of Analytical Atomic Spectrometry, Vol. 38, Issue 10 https://doi.org/10.1039/D3JA00248A	journal	January 2023
Mapping of lanthanide-tagged proteins on western blot paper using microextraction-inductively coupled plasma-mass spectrometry Stanberry, Jordan S.; Meeks, Reagan; Peterson, Ryan W. Journal of Analytical Atomic Spectrometry, Vol. 40, Issue 4 https://doi.org/10.1039/D4JA00440J	journal	January 2025
Mapping of uranium particles on J-type swipes with microextraction-ICP-MS Bradley, Veronica C.; Burleson, Jacob; Andrews, Hunter B. The Analyst, Vol. 149, Issue 8 https://doi.org/10.1039/d3an02101g	journal	January 2024
Reproducible automated renewable column generation Metzger, Shalina C.; Ticknor, Brian W.; Tevepaugh, Kayron N. Separation Science and Technology, Vol. 55, Issue 5 https://doi.org/10.1080/01496395.2019.1577439	journal	February 2019

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Round Robin Analysis of Uranium Isotopics on Cotton Swipes Measured Using Microextraction-Based Sampling Versus Conventional Bulk Analysis

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