Concomitant ion effects on isotope ratio measurements with liquid sampling – atmospheric pressure glow discharge ion source Orbitrap mass spectrometry

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

doi:10.1039/C7JA00308K

Concomitant ion effects on isotope ratio measurements with liquid sampling – atmospheric pressure glow discharge ion source Orbitrap mass spectrometry

Journal Article · Sun Dec 31 23:00:00 EST 2017 · Journal of Analytical Atomic Spectrometry

DOI:https://doi.org/10.1039/C7JA00308K· OSTI ID:1439664

^[1]; ^[2]; Hager, George J. ^[3]; Hart, Garret L. ^[3]; ^[3]

Department of Chemistry; Clemson University; Clemson; USA; EMSL
Department of Chemistry; Clemson University; Clemson; USA
EMSL; Pacific Northwest National Lab; Richland; USA

RATIONALE: The field of highly accurate and precise isotope ratio (IR) analysis has been dominated by inductively coupled plasma and thermal ionization mass spectrometers. While these instruments are considered the gold standard for IR analysis, the International Atomic Energy Agency desires a field deployable instrument capable of accurately and precisely measuring U isotope ratios.

METHODS: The proposed system interfaces the liquid sampling – atmospheric pressure glow discharge (LS-APGD) ion source with a high resolution Exactive Orbitrap mass spectrometer. With this experimental setup certified U isotope standards and unknown samples were analyzed. The accuracy and precision of the system were then determined. RESULTS: The LS-APGD /Exactive instrument measures a certified reference material of natural U (235U/238U = 0.007258) as 0.007041 with a relative standard deviation of 0.158% meeting the International Target Values for Uncertainty for the destructive analysis of U. Additionally, when three unknowns measured and compared to the results from an ICP multi collector instrument, there is no statistical difference between the two instruments.

CONCLUSIONS: The LS-APGD / Orbitrap system, while still in the preliminary stages of development, offers highly accurate and precise IR analysis that suggest a paradigm shift in the world of IR analysis. Furthermore, the portability of the LS-APGD as an elemental ion source combined with the low overhead and small size of the Orbitrap suggest that the instrumentation is capable of being field deployable.

With liquid sampling glow discharge-Orbitrap MS, isotope ratio and precision performance improves with rejection of concomitant ion species.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (US)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation (NA-20)

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1439664

Report Number(s):: PNNL-SA-124756; DN4001030

Journal Information:: Journal of Analytical Atomic Spectrometry, Journal Name: Journal of Analytical Atomic Spectrometry Journal Issue: 2 Vol. 33; ISSN JASPE2; ISSN 0267-9477

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

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