A new highly enriched 233U reference material for improved simultaneous determination of uranium amount and isotope amount ratios in trace level samples

Essex, Richard M.; Williams, Ross W.; Rogers, Kayron T.; Hexel, Cole R.; Parsons‐Davis, Tashi; Treinen, Kerri C.

doi:10.1016/j.talanta.2020.121638

Cited by 6 publications

(2 citation statements)

References 15 publications

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“…The sources of imprecision and error, throughout the measurement process, are of fundamental concern. In general, poor quantitative accuracy can be remedied using a bracketed analysis of isotopic standards to correct for what is colloquially termed “mass bias” in the case of sector-field spectrometry. , Despite this, it is pertinent to look at the effects that these parameters have on the “raw” IR accuracy. The effects of transient lengths on the accuracy of the IRs, using peak heights and peak areas are shown in upper portion of Figure using a nominal value of 8140 transient coadditions; a number yielding high-fidelity signals for the very minor isotopes as presented in Figure .…”

Section: Resultsmentioning

confidence: 99%

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

Nagornov

Kozhinov

et al. 2021

J. Am. Soc. Mass Spectrom.

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Isotope ratio (IR) analysis of natural abundance uranium presents a formidable challenge for mass spectrometry (MS): the required spectral dynamic range needs to enable the quantitatively accurate measurement of the 234UO2 species present at ∼0.0053% isotopic abundance. We address this by empowering a benchtop Orbitrap Fourier transform mass spectrometer (FTMS) coupled with the liquid sampling–atmospheric pressure glow discharge (LS-APGD) ion source and an external high-performance data acquisition system, FTMS Booster X2. The LS-APGD microplasma has demonstrated impressive capabilities regarding elemental and IR analysis when coupled with Orbitrap FTMS. Despite successes, there are limitations regarding the dynamic range and mass resolution that stem from space charge effects and data acquisition and processing restrictions. To overcome these limitations, the FTMS Booster was externally interfaced to an LS-APGD Q Exactive Focus Orbitrap FTMS to obtain time-domain signals (transients) and to process unreduced data. The unreduced time-domain data acquisition with user-controlled processing permit the evaluation of the effects of in-hardware transient phasing, increased transient lengths, advanced transient coadding, varying the length of a transient to be processed with a user-defined time increment, and the use of absorption-mode FT (aFT) processing methods on IR analysis. The added capabilities extend the spectral dynamic range of the instrument to at least 4–5 orders of magnitude and provide a resolution improvement from ∼70k to 900k m/Δm at 200 m/z. The empowered LS-APGD Orbitrap platform allows for the simultaneous measurement of 234UO2 and the prominent 235UO2 and 238UO2 isotopic species at their natural abundances, ultimately yielding improvements in performance when compared to previous uranium IR results on this same Q Exactive Focus instrument.

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Section: Resultsmentioning

confidence: 99%

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

Nagornov

Kozhinov

et al. 2021

J. Am. Soc. Mass Spectrom.

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“…High levels of precision rely on the repeatability of the sample introduction process, and the stability of the ionization source and that of the MS measurement system. Accuracy, is generally a less stringent aspect regarding the instrumentation as the use of various correction factors based on use of standard samples, can remedy nonuniform instrument responses (Mathew et al, 2013; Essex et al, 2021). Of course, this only works if the measurements themselves have a high level of precision.…”

Section: Analytical Applicationsmentioning

confidence: 99%

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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Effect of weighing uncertainty on assay values by isotope dilution mass spectrometry

Mathew

Vinai

Ottenfeld

et al. 2021

J Radioanal Nucl Chem

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A new highly enriched 233U reference material for improved simultaneous determination of uranium amount and isotope amount ratios in trace level samples

Cited by 6 publications

References 15 publications

Improved Uranium Isotope Ratio Analysis in Liquid Sampling–Atmospheric Pressure Glow Discharge/Orbitrap FTMS Coupling through the Use of an External Data Acquisition System

Improved Uranium Isotope Ratio Analysis in Liquid Sampling–Atmospheric Pressure Glow Discharge/Orbitrap FTMS Coupling through the Use of an External Data Acquisition System

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

Effect of weighing uncertainty on assay values by isotope dilution mass spectrometry

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