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

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

doi:10.1016/j.aca.2022.339836

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

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

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Abstract

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.

Original language	English
Article number	339836
Journal	Analytica Chimica Acta
Volume	1209
DOIs	https://doi.org/10.1016/j.aca.2022.339836
State	Published - May 29 2022

Funding

This work was supported by the Department of Energy's National Nuclear Security Administration under contract DE-AC05-000R22725 with UT-Batelle, LLC. Oak Ridge National Laboratory is managed by UT-Batelle for the Department of Energy under contract DE-AC-05-000R22725. The authors would like to acknowledge Jaimee Janiga (ORNL) for the assistance with graphics.

Funders	Funder number
Department of Energy's National Nuclear Security Administration
Jaimee Janiga
UT-Batelle
U.S. Department of Energy	DE-AC-05-000R22725
Oak Ridge National Laboratory

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@article{c6d7e373983f43bf94ba338c15908ae3,

title = "Direct isotopic analysis of solid uranium particulates on cotton swipes by microextraction-ICP-MS",

abstract = "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.",

author = "Bradley, {Veronica C.} and Spano, {Tyler L.} and Metzger, {Shalina C.} and Ticknor, {Brian W.} and Dunlap, {Daniel R.} and Zirakparvar, {N. Alex} and Roach, {Benjamin D.} and Hexel, {Cole R.} and Manard, {Benjamin T.}",

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T1 - Direct isotopic analysis of solid uranium particulates on cotton swipes by microextraction-ICP-MS

AU - Bradley, Veronica C.

AU - Spano, Tyler L.

AU - Metzger, Shalina C.

AU - Ticknor, Brian W.

AU - Dunlap, Daniel R.

AU - Zirakparvar, N. Alex

AU - Roach, Benjamin D.

AU - Hexel, Cole R.

AU - Manard, Benjamin T.

PY - 2022/5/29

Y1 - 2022/5/29

N2 - 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.

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

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