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Title: Preliminary Figures of Merit for Isotope Ratio Measurements: The Liquid Sampling-Atmospheric Pressure Glow Discharge Microplasma Ionization Source Coupled to an Orbitrap Mass Analyzer

ABSTRACT In order to meet a growing need for fieldable mass spectrometer systems for precise elemental and isotopic analyses, the liquid sampling-atmospheric pressure glow discharge (LS-APGD) has a number of very promising characteristics. One key set of attributes that await validation deals with the performance characteristics relative to isotope ratio precision and accuracy. Due to its availability and prior experience with this research team, the initial evaluation of isotope ratio (IR) performance was performed on a Thermo Scientific Exactive Orbitrap instrument. While the mass accuracy and resolution performance for orbitrap analyzers are very well documented, no detailed evaluations of the IR performance have been published. Efforts described here involve two variables: the inherent IR precision and accuracy delivered by the LSAPGD microplasma and the inherent IR measurement qualities of orbitrap analyzers. Important to the IR performance, the various operating parameters of the orbitrap sampling interface, HCD dissociation stage, and ion injection/data acquisition have been evaluated. The IR performance for a range of other elements, including natural, depleted, and enriched uranium isotopes was determined. In all cases the precision and accuracy are degraded when measuring low abundance (<0.1% isotope fractions). In the best case, IR precision on the order of 0.1more » %RSD can be achieved, with values of 1-3 %RSD observed for low-abundance species. The results suggest that the LSAPGD is a very good candidate for field deployable MS analysis and that the high resolving powers of the orbitrap may be complemented with a here-to-fore unknown capacity to deliver high-precision isotope ratios.« less
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Publication Date:
OSTI Identifier:
Report Number(s):
Journal ID: ISSN 1044-0305; 48439; 48771; DN4001030
DOE Contract Number:
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of the American Society for Mass Spectrometry; Journal Volume: 27; Journal Issue: 8
American Society for Mass Spectrometry
Research Org:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org:
Country of Publication:
United States
Liquid sampling-atmospheric pressure glow discharge; orbitrap mass analyzer; isotope ratio analysis; uranium; Environmental Molecular Sciences Laboratory