skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Abstract

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 themore » 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.« less

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [3]; ORCiD logo [3]
  1. Department of Chemistry; Clemson University; Clemson; USA; EMSL
  2. Department of Chemistry; Clemson University; Clemson; USA
  3. EMSL; Pacific Northwest National Lab; Richland; USA
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
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)
OSTI Identifier:
1439664
Report Number(s):
PNNL-SA-124756
Journal ID: ISSN 0267-9477; JASPE2; DN4001030
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of Analytical Atomic Spectrometry
Additional Journal Information:
Journal Volume: 33; Journal Issue: 2; Journal ID: ISSN 0267-9477
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
atmospheric pressure sampling; isotope ratio; isotope ratio analysis; isotope ratio measurements; liquid sampling-atmospheric pressure glow discharge; mass spectrometry; Orbitrap; uranium; orbitrap mass analyzer

Citation Formats

Hoegg, Edward D., Marcus, R. Kenneth, Hager, George J., Hart, Garret L., and Koppenaal, David W. Concomitant ion effects on isotope ratio measurements with liquid sampling – atmospheric pressure glow discharge ion source Orbitrap mass spectrometry. United States: N. p., 2018. Web. doi:10.1039/C7JA00308K.
Hoegg, Edward D., Marcus, R. Kenneth, Hager, George J., Hart, Garret L., & Koppenaal, David W. Concomitant ion effects on isotope ratio measurements with liquid sampling – atmospheric pressure glow discharge ion source Orbitrap mass spectrometry. United States. doi:10.1039/C7JA00308K.
Hoegg, Edward D., Marcus, R. Kenneth, Hager, George J., Hart, Garret L., and Koppenaal, David W. Mon . "Concomitant ion effects on isotope ratio measurements with liquid sampling – atmospheric pressure glow discharge ion source Orbitrap mass spectrometry". United States. doi:10.1039/C7JA00308K.
@article{osti_1439664,
title = {Concomitant ion effects on isotope ratio measurements with liquid sampling – atmospheric pressure glow discharge ion source Orbitrap mass spectrometry},
author = {Hoegg, Edward D. and Marcus, R. Kenneth and Hager, George J. and Hart, Garret L. and Koppenaal, David W.},
abstractNote = {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.},
doi = {10.1039/C7JA00308K},
journal = {Journal of Analytical Atomic Spectrometry},
issn = {0267-9477},
number = 2,
volume = 33,
place = {United States},
year = {2018},
month = {1}
}

Works referenced in this record:

Current trends: a perspective from 30 years of Atomic Spectrometry Updates
journal, January 2016

  • Butler, Owen T.; Clough, Robert; Cook, Jennifer M.
  • Journal of Analytical Atomic Spectrometry, Vol. 31, Issue 1
  • DOI: 10.1039/C5JA90056E

Spectroscopic and electrical studies of a solution-cathode glow discharge
journal, January 2005

  • Webb, Michael R.; Andrade, Francisco J.; Gamez, Gerardo
  • Journal of Analytical Atomic Spectrometry, Vol. 20, Issue 11
  • DOI: 10.1039/b503961d

Preliminary Figures of Merit for Isotope Ratio Measurements: The Liquid Sampling-Atmospheric Pressure Glow Discharge Microplasma Ionization Source Coupled to an Orbitrap Mass Analyzer
journal, April 2016

  • Hoegg, Edward D.; Barinaga, Charles J.; Hager, George J.
  • Journal of The American Society for Mass Spectrometry, Vol. 27, Issue 8
  • DOI: 10.1007/s13361-016-1402-4

Evaluation of the operating parameters of the liquid sampling-atmospheric pressure glow discharge (LS-APGD) ionization source for elemental mass spectrometry
journal, July 2014

  • Zhang, Lynn X.; Manard, Benjamin T.; Kappel, Stefanie Konegger
  • Analytical and Bioanalytical Chemistry, Vol. 406, Issue 29
  • DOI: 10.1007/s00216-014-7990-6

UV/visible Fourier transform spectroscopy using an inductively-coupled plasma: dual-channel noise cancellation
journal, April 1993

  • Travis, J. C.; Winchester, M. R.; Salit, M. L.
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 48, Issue 5
  • DOI: 10.1016/0584-8547(93)80073-4

Performance of an inductively coupled plasma source ion trap mass spectrometer
journal, January 1994

  • Koppenaal, David W.; Barinaga, Charles J.; Smith, Monty R.
  • Journal of Analytical Atomic Spectrometry, Vol. 9, Issue 9
  • DOI: 10.1039/ja9940901053

Liquid sampling-atmospheric pressure glow discharge (LS-APGD) microplasmas for diverse spectrochemical analysis applications
journal, January 2017

  • Marcus, R. Kenneth; Manard, Benjamin T.; Quarles, C. Derrick
  • Journal of Analytical Atomic Spectrometry, Vol. 32, Issue 4
  • DOI: 10.1039/C7JA00008A

Orbitrap Mass Spectrometry
journal, May 2013

  • Zubarev, Roman A.; Makarov, Alexander
  • Analytical Chemistry, Vol. 85, Issue 11
  • DOI: 10.1021/ac4001223

Accurate and precise determination of isotopic ratios by MC-ICP-MS: A review
journal, November 2009


Mass shifts and local space charge effects observed in the quadrupole ion trap at higher resolution
journal, May 1995

  • Cox, K. A.; Cleven, C. D.; Cooks, R. G.
  • International Journal of Mass Spectrometry and Ion Processes, Vol. 144, Issue 1-2
  • DOI: 10.1016/0168-1176(95)04152-B

Thermal ionisation mass spectrometry (TIMS) in nuclear science and technology – a review
journal, January 2016


Isotope ratio characteristics and sensitivity for uranium determinations using a liquid sampling-atmospheric pressure glow discharge ion source coupled to an Orbitrap mass analyzer
journal, January 2016

  • Hoegg, Edward D.; Barinaga, Charles J.; Hager, George J.
  • Journal of Analytical Atomic Spectrometry, Vol. 31, Issue 12
  • DOI: 10.1039/C6JA00163G

Space-charge effects on Fourier transform ion cyclotron resonance signals: Experimental observations and three-dimensional trajectory simulations
journal, April 1997


Frontiers of stable isotope geoscience
journal, April 2014


Ion-trap mass spectrometry with an inductively coupled plasma source
journal, January 1994

  • Barinaga, Charles J.; Koppenaal, David W.; McLuckey, Scott A.
  • Rapid Communications in Mass Spectrometry, Vol. 8, Issue 1
  • DOI: 10.1002/rcm.1290080114

Liquid Sampling-Atmospheric Pressure Glow Discharge Ionization Source for Elemental Mass Spectrometry
journal, April 2011

  • Marcus, R. Kenneth; Quarles, C. Derrick; Barinaga, Charles J.
  • Analytical Chemistry, Vol. 83, Issue 7
  • DOI: 10.1021/ac200098h

High-Resolution Inductively Coupled Plasma Fourier Transform Ion Cyclotron Resonance Mass Spectrometry
journal, September 1997

  • Milgram, K. Eric; White, Forest M.; Goodner, Kevin L.
  • Analytical Chemistry, Vol. 69, Issue 18
  • DOI: 10.1021/ac970126n

Experimental evidence for space-charge effects between ions of the same mass-to-charge in Fourier-transform ion cyclotron resonance mass spectrometry
journal, September 2007

  • Wong, Richard L.; Amster, I. Jonathan
  • International Journal of Mass Spectrometry, Vol. 265, Issue 2-3
  • DOI: 10.1016/j.ijms.2007.01.014

Determination of uranium isotope ratios using a liquid sampling atmospheric pressure glow discharge/Orbitrap mass spectrometer system
journal, August 2017

  • Hoegg, Edward D.; Marcus, R. Kenneth; Koppenaal, David W.
  • Rapid Communications in Mass Spectrometry, Vol. 31, Issue 18
  • DOI: 10.1002/rcm.7937

Liquid sampling–atmospheric pressure glow discharge (LS-APGD) ionization source for elemental mass spectrometry: preliminary parametric evaluation and figures of merit
journal, September 2011

  • Quarles, C. Derrick; Carado, Anthony J.; Barinaga, Charles J.
  • Analytical and Bioanalytical Chemistry, Vol. 402, Issue 1
  • DOI: 10.1007/s00216-011-5359-7

Space charge effects on relative peak heights in fourier transform-ion cyclotron resonance spectra
journal, October 1992


An Atmospheric Pressure Glow Discharge Optical Emission Source for the Direct Sampling of Liquid Media
journal, July 2001

  • Marcus, R. Kenneth; Davis, W. Clay
  • Analytical Chemistry, Vol. 73, Issue 13
  • DOI: 10.1021/ac010158h

Application of mathematical procedures to background correction and multivariate analysis in inductively coupled plasma-optical emission spectrometry
journal, May 1998

  • van Veen, E. H.; de Loos-Vollebregt, M. T. C.
  • Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 53, Issue 5
  • DOI: 10.1016/S0584-8547(98)00109-8

Analysis of molecular isotopic structures at high precision and accuracy by Orbitrap mass spectrometry
journal, November 2017


Performance of Orbitrap Mass Analyzer at Various Space Charge and Non-Ideal Field Conditions: Simulation Approach
journal, February 2012

  • Kharchenko, Andriy; Vladimirov, Gleb; Heeren, Ron M. A.
  • Journal of The American Society for Mass Spectrometry, Vol. 23, Issue 5
  • DOI: 10.1007/s13361-011-0325-3