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Title: Atmospheric-pressure ionization and fragmentation of peptides by solution-cathode glow discharge

Abstract

Modern “-omics” (e.g., proteomics, glycomics, metabolomics, etc.) analyses rely heavily on electrospray ionization and tandem mass spectrometry to determine the structural identity of target species. Unfortunately, these methods are limited to specialized mass spectrometry instrumentation. Here in this paper, a novel approach is described that enables ionization and controlled, tunable fragmentation of peptides at atmospheric pressure. In the new source, a direct-current plasma is sustained between a tapered metal rod and a flowing sample-containing solution. As the liquid stream contacts the electrical discharge, peptides from the solution are volatilized, ionized, and fragmented. At high discharge currents (e.g., 70 mA), electrospray-like spectra are observed, dominated by singly and doubly protonated molecular ions. At lower currents (35 mA), many peptides exhibit extensive fragmentation, with a-, b-, c-, x-, and y-type ion series present as well as complex fragments, such as d-type ions, not previously observed with atmospheric-pressure dissociation. Though the mechanism of fragmentation is currently unclear, observations indicate it could result from the interaction of peptides with gas-phase radicals or ultraviolet radiation generated within the plasma.

Authors:
 [1];  [2];  [2];  [2];  [1]
+ Show Author Affiliations
  1. Indiana Univ., Bloomington, IN (United States). Dept. of Chemistry
  2. Kent State Univ., Kent, OH (United States). Dept. of Chemistry and Biochemistry
Publication Date:
Research Org.:
Indiana Univ., Bloomington, IN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1421367
Grant/Contract Number:  
FG02-98ER14890
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Science
Additional Journal Information:
Journal Volume: 7; Journal Issue: 10; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Schwartz, Andrew J., Shelley, Jacob T., Walton, Courtney L., Williams, Kelsey L., and Hieftje, Gary M. Atmospheric-pressure ionization and fragmentation of peptides by solution-cathode glow discharge. United States: N. p., 2016. Web. doi:10.1039/c6sc02032a.
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Schwartz, Andrew J., Shelley, Jacob T., Walton, Courtney L., Williams, Kelsey L., & Hieftje, Gary M. Atmospheric-pressure ionization and fragmentation of peptides by solution-cathode glow discharge. United States. https://doi.org/10.1039/c6sc02032a
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Schwartz, Andrew J., Shelley, Jacob T., Walton, Courtney L., Williams, Kelsey L., and Hieftje, Gary M. Mon . "Atmospheric-pressure ionization and fragmentation of peptides by solution-cathode glow discharge". United States. https://doi.org/10.1039/c6sc02032a. https://www.osti.gov/servlets/purl/1421367.
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@article{osti_1421367,
title = {Atmospheric-pressure ionization and fragmentation of peptides by solution-cathode glow discharge},
author = {Schwartz, Andrew J. and Shelley, Jacob T. and Walton, Courtney L. and Williams, Kelsey L. and Hieftje, Gary M.},
abstractNote = {Modern “-omics” (e.g., proteomics, glycomics, metabolomics, etc.) analyses rely heavily on electrospray ionization and tandem mass spectrometry to determine the structural identity of target species. Unfortunately, these methods are limited to specialized mass spectrometry instrumentation. Here in this paper, a novel approach is described that enables ionization and controlled, tunable fragmentation of peptides at atmospheric pressure. In the new source, a direct-current plasma is sustained between a tapered metal rod and a flowing sample-containing solution. As the liquid stream contacts the electrical discharge, peptides from the solution are volatilized, ionized, and fragmented. At high discharge currents (e.g., 70 mA), electrospray-like spectra are observed, dominated by singly and doubly protonated molecular ions. At lower currents (35 mA), many peptides exhibit extensive fragmentation, with a-, b-, c-, x-, and y-type ion series present as well as complex fragments, such as d-type ions, not previously observed with atmospheric-pressure dissociation. Though the mechanism of fragmentation is currently unclear, observations indicate it could result from the interaction of peptides with gas-phase radicals or ultraviolet radiation generated within the plasma.},
doi = {10.1039/c6sc02032a},
journal = {Chemical Science},
number = 10,
volume = 7,
place = {United States},
year = {Mon Jun 27 00:00:00 EDT 2016},
month = {Mon Jun 27 00:00:00 EDT 2016}
}
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Publisher's Version of Record
https://doi.org/10.1039/c6sc02032a
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