Determination of uranium isotope ratios using a liquid sampling atmospheric pressure glow discharge/Orbitrap mass spectrometer system

Hoegg, Edward D.; Marcus, R. Kenneth; Koppenaal, David W.; Irvahn, Jan; Hager, George J.; Hart, Garret L.

doi:10.1002/rcm.7937

Cited by 22 publications

(30 citation statements)

References 13 publications

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“…The LS‐APGD coupled to an Orbitrap mass spectrometer was the first of these new hybrid sources to measure uranium isotope ratios (Hoegg et al, 2016). After optimization of source and MS conditions, the LS‐APGD was reported to produce uranium isotope‐ratio precisions of 0.04% RSD for highly enriched uranium at 80% 235 U (Hoegg et al, 2019b, 2017, 2016). The SCGD‐MS combination has also been tested for the measurement of uranium isotope ratios (Maclean, Chan, & Shelley, 2018).…”

Section: Hybrid Organic/elemental Ionization Sourcesmentioning

confidence: 99%

Modern Plasma‐based Desorption/Ionization: From Atoms and Molecules to Chemical Synthesis

Molnar

Shelley

2020

Mass Spectrometry Reviews

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Since the first mass spectrometry (MS) experiments were conducted by Thomson and Aston, plasmas have been used as ionization sources. Historically, plasma ion sources were used for these experiments because they were one of the few known sources of gasphase ions at the time and they were relatively simple to setup and operate. Since then, developments in plasma ionization have continued to inform and motivate advances in other areas of MS. For example, plasma-desorption MS demonstrated ionization of large peptides and polymers more than 10 years before the first descriptions of electrospray ionization (ESI) and matrix-assisted laser desorption/ionization (MALDI). As a result, significant effort was placed on development of ionization approaches, mass analysis, and detection approaches for very large molecules: even before the advent of ESI and MALDI. Since then, new analytical challenges and opportunities in plasma ionization have arisen. In this review, the emerging trends in plasma-based ionization for several areas of MS will be discussed, including molecular ionization, elemental ionization, hybrid elemental and molecular ion sources, and unique chemical transformations.

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Section: Hybrid Organic/elemental Ionization Sourcesmentioning

confidence: 99%

Modern Plasma‐based Desorption/Ionization: From Atoms and Molecules to Chemical Synthesis

Molnar

Shelley

2020

Mass Spectrometry Reviews

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“…Because of the aforementioned software glitch, the reported accuracy in 235 U/ 238 U ratio measurements should not be taken as representative and significant improvement is anticipated once the software bug is fixed. At present, the researchers evaluated the analytical accuracy through a correction scaling factor [16,131]. In their latest report [131], the researchers determined this scaling factor through a certified reference material of natural U, and measured the 235 U/ 238 U ratios of three unknown natural-U samples.…”

Section: Liquid Sampling-atmospheric Pressure Glow Discharge (Ls-apgd) Mass Spectrometrymentioning

confidence: 99%

“…At present, the researchers evaluated the analytical accuracy through a correction scaling factor [16,131]. In their latest report [131], the researchers determined this scaling factor through a certified reference material of natural U, and measured the 235 U/ 238 U ratios of three unknown natural-U samples. With cross validation with multicollector-ICP-MS, it was reported that there was no statistical difference in the determined 235 U/ 238 U ratios from the two instruments (i.e., LS-APGD-MS and MC-ICP-MS) [131].…”

Section: Liquid Sampling-atmospheric Pressure Glow Discharge (Ls-apgd) Mass Spectrometrymentioning

confidence: 99%

“…In their latest report [131], the researchers determined this scaling factor through a certified reference material of natural U, and measured the 235 U/ 238 U ratios of three unknown natural-U samples. With cross validation with multicollector-ICP-MS, it was reported that there was no statistical difference in the determined 235 U/ 238 U ratios from the two instruments (i.e., LS-APGD-MS and MC-ICP-MS) [131]. However, it has been stated that this correction scaling factor depends on the 235 U/ 238 U ratio, as well as a change every time that the system is restarted [131].…”

Section: Liquid Sampling-atmospheric Pressure Glow Discharge (Ls-apgd) Mass Spectrometrymentioning

confidence: 99%

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Scoping study to expedite development of a field deployable and portable instrument for UF6 enrichment assay

Chan¹,

Valentine²,

Russo³

2017

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The primary objective of the present study is to identity the most promising, viable technologies that are likely to culminate in an expedited development of the next-generation, field-deployable instrument for providing rapid, accurate, and precise enrichment assay of uranium hexafluoride (UF 6 ). UF 6 is typically involved, and is arguably the most important uranium compound, in uranium enrichment processes. As the first line of defense against proliferation, accurate analytical techniques to determine the uranium isotopic distribution in UF 6 are critical for materials verification, accounting, and safeguards at enrichment plants. As nuclear fuel cycle technology becomes more prevalent around the world, international nuclear safeguards and interest in UF 6 enrichment assay has been growing.At present, laboratory-based mass spectrometry (MS), which offers the highest attainable analytical accuracy and precision, is the technique of choice for the analysis of stable and longlived isotopes. Currently, the International Atomic Energy Agency (IAEA) monitors the production of enriched UF 6 at declared facilities by collecting a small amount (between 1 to 10 g) of gaseous UF 6 into a sample bottle, which is then shipped under chain of custody to a central laboratory (IAEA's Nuclear Materials Analysis Laboratory) for high-precision isotopic assay by MS. The logistics are cumbersome and new shipping regulations are making it more difficult to transport UF 6 . Furthermore, the analysis is costly, and results are not available for some time after sample collection. Hence, the IAEA is challenged to develop effective safeguards approaches at enrichment plants. In-field isotopic analysis of UF 6 has the potential to substantially reduce the time, logistics and expense of sample handling. However, current laboratory-based MS techniques require too much infrastructure and operator expertise for field deployment and operation. As outlined in the IAEA Department of Safeguards Long-Term R&D Plan, 2012-2023, one of the IAEA long-term R&D needs is to "develop tools and techniques to enable timely, potentially real-time, detection of HEU (Highly Enriched Uranium) production in LEU (Lowly Enriched Uranium) enrichment facilities" (Milestone 5.2). iv measurements that do not require the stated high accuracy or precision of the ITVs to which it was compared).The list presented below summarizes the outcome of the present study, and groups all reviewed techniques into "recommended", "promising", or "not recommended"; the "benchmark" techniques are also included and labeled as such. The list is presented in a highly abridged way such that only the final recommendations are given. The performance of a technique in the seven evaluation metrics and its ranking are summarized in Table 6.1, whereas short discussion and comments on the recommendation can be found in Section 6.2 of this report. Furthermore, comprehensive and in-depth reviews on the scientific principle of each technique, its instrument option, its limitations and main gaps betwe...

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“…1, 2 As technologies improve, it is important to evaluate state-of-the-art mass spectrometry (MS) approaches for these aims. As such, the analytical performance of a wide range of isotope ratio (IR)MS-based instrumentation and techniques have been investigated, including secondary ion mass spectrometry (SIMS), 3-10 thermal ionization (TI)MS, 11,12 inductively coupled plasma (ICP)-MS, 13,14 , isotope dilution (ID)MS, 15 extractive electrospray ionization (EESI)-MS, 16, 17 and atmospheric plasma-based sources such as microwave plasma torch (MPT)-MS, 18 solution-cathode glow discharge (SCGD), 19 and liquid sampling-atmospheric pressure glow discharge (LS- APGD) ionization coupled with Orbitrap MS. 20-23…”

Section: Introductionmentioning

confidence: 99%

Considerations for uranium isotope ratio analysis by atmospheric pressure ionization mass spectrometry

Forbes

Szakal

2019

Analyst

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The accurate measurement of uranium isotope ratios from trace samples lies at the foundation of achieving nuclear nonproliferation. These challenging measurements necessitate both the continued characterization and evaluation of evolving mass spectrometric technologies as well as the propagation of sound measurement approaches. For the first time in this work, we present the analysis of uranium isotope ratio measurements from discrete liquid injections with an ultra- high-resolution hybrid quadrupole time-of-flight mass spectrometer. Also presented are important measurement considerations for evaluating the performance of this type and other atmospheric pressure and ambient ionization mass spectrometers for uranium isotope analysis. Specifically, as the goal of achieving isotope ratios from as little as a single picogram of solid material is approached, factors such as mass spectral sampling rate, collision induced dissociation (CID) potentials, and mass resolution can dramatically alter the measured isotope ratio as a function of mass loading. We present the ability to accurately measure 235UO2+238UO2+ down to 10’s of picograms of solubilized uranium oxide through a proper consideration of mass spectral parameters while identifying limitations and opportunities for pushing this limit further.

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Determination of uranium isotope ratios using a liquid sampling atmospheric pressure glow discharge/Orbitrap mass spectrometer system

Cited by 22 publications

References 13 publications

Modern Plasma‐based Desorption/Ionization: From Atoms and Molecules to Chemical Synthesis

Modern Plasma‐based Desorption/Ionization: From Atoms and Molecules to Chemical Synthesis

Scoping study to expedite development of a field deployable and portable instrument for UF6 enrichment assay

Considerations for uranium isotope ratio analysis by atmospheric pressure ionization mass spectrometry

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