Fragmentation of Singly, Doubly, and Triply Charged Hydrogen Deficient Peptide Radical Cations in Infrared Multiphoton Dissociation and Electron Induced Dissociation

Kalli, Anastasia; Hess, Sonja

doi:10.1007/s13361-011-0272-z

Cited by 14 publications

(26 citation statements)

References 76 publications

(196 reference statements)

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“…EID is believed to occur via both electronic and vibrational excitation [53]. [21]. The b 8 was only observed for the even electron species (data not shown), whereas the y 9 and y 3 were only detected for the hydrogen-deficient species [21].…”

Section: Ecd Of Triply Charged Radical Cationsmentioning

confidence: 94%

“…Formation of a-, b-, c-, y-, x-, and ztype product ions along with side chain losses were observed [5,16,[20][21][22].…”

Section: Dissociation Of Doubly [M + H] 2+• and Triply [M + 2h] 3+mentioning

confidence: 94%

“…• , charged species has also been examined [5,16,[20][21][22]. Formation of a-, b-, c-, y-, x-, and ztype product ions along with side chain losses were observed [5,16,[20][21][22].…”

Section: Dissociation Of Doubly [M + H] 2+• and Triply [M + 2h] 3+mentioning

confidence: 98%

“…These experiments aim to address whether the presence of a hydrogen-deficient radical site influences the ECD outcome. In addition, dissociation pathways of hydrogen-deficient species have been characterized in CID [5,11,13,15,16,18,20,[22][23][24], infrared multiphoton dissociation (IRMPD) [21], and electron-induced dissociation (EID) [21]. However, they have not been so far investigated in ECD.…”

Section: Dissociation Of Doubly [M + H] 2+• and Triply [M + 2h] 3+mentioning

confidence: 99%

“…The vast majority of the b-and y-ions detected for [Ile 7 ]-angiotensin III should originate from the excited [M + 2H] 2+* species since such ions were either of very low abundance or absent in the CID, IRMPD, and EID spectra of the M +• precursor ions [21]. EID is believed to occur via both electronic and vibrational excitation [53].…”

Section: Ecd Of Triply Charged Radical Cationsmentioning

confidence: 99%

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Electron Capture Dissociation of Hydrogen-Deficient Peptide Radical Cations

Kalli

Hess

2012

J. Am. Soc. Mass Spectrom.

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Hydrogen-deficient peptide radical cations exhibit fascinating gas phase chemistry, which is governed by radical driven dissociation and, in many cases, by a combination of radical and charge driven fragmentation. Here we examine electron capture dissociation (ECD) of doubly, • precursor ions resulted in efficient electron capture by the hydrogen-deficient species. However, the intensities of c-and z-type product ions were reduced, compared with those observed for the even electron species, indicating suppression of N-C α backbone bond cleavages. We postulate that radical recombination occurs after the initial electron capture event leading to a stable even electron intermediate, which does not trigger N-C α bond dissociations. Although the intensities of c-and z-type product ions were reduced, the number of backbone bond cleavages remained largely unaffected between the ECD spectra of the even electron and hydrogen-deficient species. We hypothesize that a small ion population exist as a biradical, which can trigger N-C α bond cleavages. Alternatively, radical recombination and N-C α bond cleavages can be in competition, with radical recombination being the dominant pathway and N-C α cleavages occurring to a lesser degree. Formation of b-and y-type ions observed for two of the hydrogendeficient peptides examined is also discussed.

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Section: Ecd Of Triply Charged Radical Cationsmentioning

confidence: 94%

“…Formation of a-, b-, c-, y-, x-, and ztype product ions along with side chain losses were observed [5,16,[20][21][22].…”

Section: Dissociation Of Doubly [M + H] 2+• and Triply [M + 2h] 3+mentioning

confidence: 94%

“…• , charged species has also been examined [5,16,[20][21][22]. Formation of a-, b-, c-, y-, x-, and ztype product ions along with side chain losses were observed [5,16,[20][21][22].…”

Section: Dissociation Of Doubly [M + H] 2+• and Triply [M + 2h] 3+mentioning

confidence: 98%

Section: Dissociation Of Doubly [M + H] 2+• and Triply [M + 2h] 3+mentioning

confidence: 99%

Section: Ecd Of Triply Charged Radical Cationsmentioning

confidence: 99%

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Electron Capture Dissociation of Hydrogen-Deficient Peptide Radical Cations

Kalli

Hess

2012

J. Am. Soc. Mass Spectrom.

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Electron‐induced dissociation (EID) for structure characterization of glycerophosphatidylcholine: determination of double‐bond positions and localization of acyl chains

Jones¹,

Thompson²,

Carter³

et al. 2015

J. Mass Spectrom.

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Mass spectrometry continues to drive the field of lipidomics across many areas of research because of its unique capability for characterizing lipids. With an accurate molecular weight, often in combination with ion mobility or liquid chromatography, MS can deconstruct a complex mixture of lipids into a table of lipid species annotated by class and isobar. Tandem MS, typically low energy CID, can further distinguish isobars by the different fatty acid fragments and in some cases reveal the fatty acid bonding position. In the Special Feature Kane and coworkers at University of Maryland apply a new electron‐induced dissociation technique to singly‐charged mono‐ and di‐unsaturated phospholipids and show how the resulting fragmentation patterns indicate the fatty acid position as well as the double bond location.

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Electron‐induced dissociation (EID) for structure characterization of glycerophosphatidylcholine: determination of double‐bond positions and localization of acyl chains

et al. 2015

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Glycerophospholipids are a highly abundant and diverse collection of biologically relevant lipids and distinction between isomeric and isobaric species is a fundamental aspect for confident identification. The ability to confidently assign a unique structure to a glycerophospholipid of interest is dependent on determining the number and location of the points of unsaturation and assignment of acyl chain position. The use of high energy electrons (>20 eV) to induce gas-phase dissociation of intact precursor ions results in diagnostic product ions for localizing double bond positions and determining acyl chain assignment. We describe a high resolution, tandem mass spectrometry method for structure characterization of glycerophospholipids using electron-induced dissociation (EID). Furthermore, the inclusion of nomenclature to systematically assign bond cleavage sites with acyl chain position and double bond location enables a uniform platform for lipid identification. The EID methodology detailed here combines novel application of an electron-based dissociation technique with high resolution mass spectrometry that facilitates a new experimental approach for lipid biomarker discovery and validation.

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Fragmentation of Singly, Doubly, and Triply Charged Hydrogen Deficient Peptide Radical Cations in Infrared Multiphoton Dissociation and Electron Induced Dissociation

Cited by 14 publications

References 76 publications

Electron Capture Dissociation of Hydrogen-Deficient Peptide Radical Cations

Electron Capture Dissociation of Hydrogen-Deficient Peptide Radical Cations

Electron‐induced dissociation (EID) for structure characterization of glycerophosphatidylcholine: determination of double‐bond positions and localization of acyl chains

Electron‐induced dissociation (EID) for structure characterization of glycerophosphatidylcholine: determination of double‐bond positions and localization of acyl chains

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