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Title: Ultra-High Resolution Elemental/Isotopic Mass Spectrometry (m/?m> 1,000,000): Coupling of the Liquid Sampling-Atmospheric Pressure Glow Discharge with an Orbitrap Mass Spectrometer for Applications in Biological Chemistry and Environmental Analysis

Abstract

Many fundamental questions of astrophysics, biochemistry, and geology rely on the ability to accurately and precisely measure the mass and abundance of isotopes. Taken a step further, the capacity to perform such measurements on intact molecules provides insights into processes in diverse biological systems. Described here is the coupling of a combined atomic and molecular (CAM) ionization source, the liquid sampling-atmospheric pressure glow discharge (LS-APGD) microplasma, with a commercially available ThermoScientific Fusion Lumos mass spectrometer. Demonstrated for the first time is the ionization and isotopically-resolved fingerprinting of a long-postulated, but never mass-spectrometrically observed, bi-metallic complex Hg:Se-cysteine. Such a complex has been implicated as having a role in observations of Hg detoxification by selenoproteins/amino acids. Demonstrated as well is the ability to mass spectrometrically-resolve the geochronologically important isobaric 87Sr and 87Rb species (?m ~ 0.3 mDa, mass resolution m/?m ? 1,700,000). The mass difference in this case reflects the beta-decay of the 87Rb to the stable Sr isotope. These two demonstrations highlight what may be a significant change in bioinorganic and atomic mass spectrometry, with impact expected across a broad spectrum of the physical, biological and geological sciences.

Authors:
 [1];  [2];  [3];  [4];  [1];  [5]
  1. BATTELLE (PACIFIC NW LAB)
  2. CNRS, Institute for Analytical and Physical Chemistry of the Environment and Materials
  3. CNRS, Institute of Analytical and Physical Chemistry of the Environment and Materials
  4. CNRS Institute for Anaylitical and Physical Chemistry of the Environment and Materials
  5. CLEMSON UNIVERSITY
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1567186
Report Number(s):
PNNL-SA-140817
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of the American Society for Mass Spectrometry
Additional Journal Information:
Journal Volume: 30; Journal Issue: 7
Country of Publication:
United States
Language:
English

Citation Formats

Hoegg, Edward D., Godin, Simon, Szpunar, Joanna, Lobinski, Ryszard, Koppenaal, David W., and Marcus, Richard K. Ultra-High Resolution Elemental/Isotopic Mass Spectrometry (m/?m> 1,000,000): Coupling of the Liquid Sampling-Atmospheric Pressure Glow Discharge with an Orbitrap Mass Spectrometer for Applications in Biological Chemistry and Environmental Analysis. United States: N. p., 2019. Web. doi:10.1007/s13361-019-02183-w.
Hoegg, Edward D., Godin, Simon, Szpunar, Joanna, Lobinski, Ryszard, Koppenaal, David W., & Marcus, Richard K. Ultra-High Resolution Elemental/Isotopic Mass Spectrometry (m/?m> 1,000,000): Coupling of the Liquid Sampling-Atmospheric Pressure Glow Discharge with an Orbitrap Mass Spectrometer for Applications in Biological Chemistry and Environmental Analysis. United States. doi:10.1007/s13361-019-02183-w.
Hoegg, Edward D., Godin, Simon, Szpunar, Joanna, Lobinski, Ryszard, Koppenaal, David W., and Marcus, Richard K. Wed . "Ultra-High Resolution Elemental/Isotopic Mass Spectrometry (m/?m> 1,000,000): Coupling of the Liquid Sampling-Atmospheric Pressure Glow Discharge with an Orbitrap Mass Spectrometer for Applications in Biological Chemistry and Environmental Analysis". United States. doi:10.1007/s13361-019-02183-w.
@article{osti_1567186,
title = {Ultra-High Resolution Elemental/Isotopic Mass Spectrometry (m/?m> 1,000,000): Coupling of the Liquid Sampling-Atmospheric Pressure Glow Discharge with an Orbitrap Mass Spectrometer for Applications in Biological Chemistry and Environmental Analysis},
author = {Hoegg, Edward D. and Godin, Simon and Szpunar, Joanna and Lobinski, Ryszard and Koppenaal, David W. and Marcus, Richard K.},
abstractNote = {Many fundamental questions of astrophysics, biochemistry, and geology rely on the ability to accurately and precisely measure the mass and abundance of isotopes. Taken a step further, the capacity to perform such measurements on intact molecules provides insights into processes in diverse biological systems. Described here is the coupling of a combined atomic and molecular (CAM) ionization source, the liquid sampling-atmospheric pressure glow discharge (LS-APGD) microplasma, with a commercially available ThermoScientific Fusion Lumos mass spectrometer. Demonstrated for the first time is the ionization and isotopically-resolved fingerprinting of a long-postulated, but never mass-spectrometrically observed, bi-metallic complex Hg:Se-cysteine. Such a complex has been implicated as having a role in observations of Hg detoxification by selenoproteins/amino acids. Demonstrated as well is the ability to mass spectrometrically-resolve the geochronologically important isobaric 87Sr and 87Rb species (?m ~ 0.3 mDa, mass resolution m/?m ? 1,700,000). The mass difference in this case reflects the beta-decay of the 87Rb to the stable Sr isotope. These two demonstrations highlight what may be a significant change in bioinorganic and atomic mass spectrometry, with impact expected across a broad spectrum of the physical, biological and geological sciences.},
doi = {10.1007/s13361-019-02183-w},
journal = {Journal of the American Society for Mass Spectrometry},
number = 7,
volume = 30,
place = {United States},
year = {2019},
month = {7}
}