Direct isotopic analysis of solid uranium particulates on cotton swipes by microextraction-ICP-MS

Bradley, Veronica; Spano, Tyler; Metzger, Shalina; Ticknor, Brian; Dunlap, Daniel; Zirakparvar, N; Roach, Benjamin; Hexel, Cole; Manard, Benjamin

doi:10.1016/j.aca.2022.339836

Title: Direct isotopic analysis of solid uranium particulates on cotton swipes by microextraction-ICP-MS

Journal Article · Sat Apr 23 00:00:00 EDT 2022 · Analytica Chimica Acta

DOI:https://doi.org/10.1016/j.aca.2022.339836· OSTI ID:1870236

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Missouri, Columbia, MO (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Direct isotope ratio analysis of solid uranium particulates on cotton swipes was achieved using a solution-based microextraction technique, coupled to a quadrupole inductively coupled plasma - mass spectrometer (ICP-MS). This microextraction-ICP-MS methodology provides rapid isotopic analysis which could be applicable to nuclear safeguards measurements. Particulates of uranyl nitrate hexahydrate (UO₂(NO₃)₂·6H₂O) and uranyl fluoride (UO₂F₂) ranging from 6 μm to 40 μm in length were transferred to cotton swipes with a particle manipulator. The microextraction probe then delivers a 5% nitric acid (HNO3) solvent onto the swipe surface to extract the uranium species. The extracted sample is then delivered to the ICP-MS for isotopic determination. The majority of uranium signal (~99% and ~94% for UO2(NO3)2·6H2O and UO₂F₂, respectively) was detected in the first 15 s extraction, while subsequent extractions on the same location had low or no U signal, suggesting near complete removal of the solid uranium compounds from the swipe surface. Ten samples (for each of the uranium compounds), were analyzed for their isotopic composition. For UO₂(NO₃)₂·6H₂O, the determined isotope ratios resulted in a % relative difference (% RD) from the referenced isotope ratios of 0.97, 1.0, and 7.3% for ²³⁴U/²³⁸U, ²³⁵U/²³⁸U, and ²³⁶U/²³⁸U, respectively. The % RD of the UO₂F₂ isotope ratios were 1.9 and 0.60% for ²³⁴U/²³⁸U and ²³⁵U/²³⁸U, respectively. The preliminary limits of detection were determined to be 0.002, 0.4, and 60 pg for ²³⁴U, ²³⁵U and ²³⁸U, respectively This work demonstrates that microextraction ICP-MS is a rapid and sensitive method that could directly determine uranium isotope ratios of UO₂(NO₃)₂·6H₂O and UO₂F₂ particulates on cotton swipes.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1870236

Journal Information:: Analytica Chimica Acta, Vol. 1209, Issue 1; ISSN 0003-2670

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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