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.; Bills, Jacob R.; Hall, Katja A.; Bostick, D.T.; Cable-Dunlap, Paula; Marcus, R. Kenneth

doi:10.1021/acs.analchem.0c01606

Cited by 21 publications

(28 citation statements)

References 48 publications

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“…After each extraction, a burp of gas (N 2 , ultrahigh purity, Airgas, Radnor, PA) was utilized to remove any debris that could be present on the probe head. The extraction solvent employed here was 2% HNO 3 , which has previously been shown to be an effective solvent for extracting uranium from a swipe surface . The flow rate of the extraction solvent through the probe head, which is also the rate entering the ICP nebulizer, was determined to be 200 μL min –1 and is driven by an isocratic liquid chromatography (LC) pump (Advion).…”

Section: Methodssupporting

confidence: 90%

“…The longer extractions times, 20, 30, 40, and 50 s, all exhibit very similar (within uncertainty) peak heights, demonstrating nearly complete analyte extraction from the site. This is similar to results reported by Marcus et al, in which peak areas did not change with longer extraction times . Elution profiles from the 5, 10, and 20 s extractions exhibit a smooth Gaussian-shaped profile, while at the longer times (30, 40, and 50 s), peak tailing is more pronounced.…”

Section: Resultsmentioning

confidence: 99%

“…This is similar to results reported by Marcus et al, in which peak areas did not change with longer extraction times. 27 Elution profiles from the 5, 10, and 20 s extractions exhibit a smooth Gaussian-shaped profile, while at the longer times (30, 40, and 50 s), peak tailing is more pronounced. This increased tailing is likely due to the wicking of uranium from the outside profile of the probe head into the extraction region.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…The extraction solvent employed here was 2% HNO 3 , which has previously been shown to be an effective solvent for extracting uranium from a swipe surface. 27 The flow rate of the extraction solvent through the probe head, which is also the rate entering the ICP nebulizer, was determined to be 200 μL min −1 and is driven by an isocratic liquid chromatography (LC) pump (Advion). The extraction solvent flow rate was determined based on the ICP-MS tune parameters for optimal sensitivity.…”

Section: ■ Experimental Sectionmentioning

confidence: 91%

“…This may allow for differentiation of multiple distributions of uranium particulates with different enrichments collected on the swipe, which is not currently possible with bulk analysis methodologies and requires particle-specific analytical techniques. Similar work was performed by Marcus et al, in which the microextraction probe was coupled to a unique ionization source for elemental analysis, the liquid sampling-atmospheric pressure glow discharge (LS-APGD) 26 coupled to an Orbitrap MS. 27 Preliminary studies, with the LS-APGD-Orbitrap MS, were able to extract ∼100 ng of uranium from the surface of a cotton swipe and provide results with a <10% relative difference and a <5% relative standard deviation between samples of known isotopic abundances. The work presented here is the first coupling of the microextraction probe to ICP-MS and provides preliminary figures-of-merit for sensitivity, precision, and accuracy for the isotopic analysis of uranium directly extracted from a swipe surface.…”

Section: ■ Introductionmentioning

confidence: 99%

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Direct Uranium Isotopic Analysis of Swipe Surfaces by Microextraction-ICP-MS

et al. 2021

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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 mm 2 ) are dissolved and extracted into a flowing solvent of 2% nitric acid (HNO 3 ). 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 238 U. Additionally, precise and accurate isotope ratio measurements were achieved on uranium reference materials for both the major ( 235 U/ 238 U) and minor ( 234 U/ 238 U and 236 U/ 238 U) 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.

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Section: Methodssupporting

confidence: 90%

Section: Resultsmentioning

confidence: 99%

Section: ■ Results and Discussionmentioning

confidence: 99%

Section: ■ Experimental Sectionmentioning

confidence: 91%

Section: ■ Introductionmentioning

confidence: 99%

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Direct Uranium Isotopic Analysis of Swipe Surfaces by Microextraction-ICP-MS

et al. 2021

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Direct sub‐atmospheric pressure ionization mass spectrometry: Evaporation/sublimation‐driven ionization is amazing, fundamentally, and practically

Trimpin,

Inutan,

Pagnotti

et al. 2024

J Mass Spectrom

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This paper covers direct sub‐atmospheric pressure ionization mass spectrometry (MS). The discovery, applications, and mechanistic aspects of novel ionization processes for use in MS that are not based on the high‐energy input from voltage, laser, and/or high temperature but on sublimation/evaporation within a region linking a higher to lower pressure and modulated by heat and collisions, are discussed, including how this new reality has guided a series of discoveries, instrument developments, and commercialization. A research focus, inter alia, is on how best to understand, improve, and use these novel ionization processes, which convert volatile and nonvolatile compounds from solids (sublimation) or liquids (evaporation) into gas‐phase ions for analysis by MS providing reproducible, accurate, sensitive, and prompt results. Our perception on how these unprecedented versus traditional ionization processes/methods relate to each other, how they can be made to coexist on the same mass spectrometer, and an outlook on new and expanded applications (e.g., clinical, portable, fast, safe, and autonomous) is presented, and is based on ST's Opening lecture presentation at the Nordic Mass spectrometry Conference, Geilo, Norway, January 2023. Focus will be on matrix‐assisted ionization (MAI) and solvent‐assisted ionization (SAI) MS covering the period from 2010 to 2023; a potential paradigm shift in the making.

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Combined atomic and molecular (CAM) ionization with the liquid sampling‐atmospheric pressure glow discharge microplasma

Marcus

Hoegg

Hall

et al. 2021

Mass Spectrometry Reviews

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In a world where information‐rich methods of analysis are often sought over those with superior figures of merit, there is a constant search for ionization methods which can be applied across diverse analytical systems. The liquid sampling‐atmospheric pressure glow discharge (LS‐APGD) is a microplasma device which has the inherent capabilities to operate as a combined atomic and molecular (CAM) ionization source. The plasma is sustained by placement of a high voltage (~500 V, dc) onto an electrolytic solution through which the analyte is generally delivered to the discharge. Judicious choice of the solvent provides a means of obtaining atomic/elemental and/or molecular mass spectra. Presented here are the diverse modes of sample introduction and mass spectrometer platforms to which the LS‐APGD has been interfaced. Likewise, representative spectra and figures of merit are presented towards elemental and isotope ratio measurements, as well as application to small organic molecules, organometallic complexes, and intact proteins. It is believed that the diversity of analytical applications and ready implementation across the entirety of mass spectrometry platforms portends a level of versatility not realized with other ionization sources.

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Rapid Determination of Uranium Isotopic Abundance from Cotton Swipes: Direct Extraction via a Planar Surface Reader and Coupling to a Microplasma Ionization Source

Cited by 21 publications

References 48 publications

Direct Uranium Isotopic Analysis of Swipe Surfaces by Microextraction-ICP-MS

Direct Uranium Isotopic Analysis of Swipe Surfaces by Microextraction-ICP-MS

Direct sub‐atmospheric pressure ionization mass spectrometry: Evaporation/sublimation‐driven ionization is amazing, fundamentally, and practically

Combined atomic and molecular (CAM) ionization with the liquid sampling‐atmospheric pressure glow discharge microplasma

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