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Please use this identifier to cite or link to this item: http://hdl.handle.net/1942/23274

Title: Conformational Space and Stability of ETD Charge Reduction Products of Ubiquitin
Authors: Lermyte, Frederik
Łącki, Mateusz Krzysztof
Valkenborg, Dirk
Gambin, Anna
Sobott, Frank
Issue Date: 2017
Publisher: SPRINGER
Abstract: Owing to its versatility, electron transfer dissociation (ETD) has become one of the most commonly utilized fragmentation techniques in both native and non-native top-down mass spectrometry. However, several competing reactions-primarily different forms of charge reduction-occur under ETD conditions, as evidenced by the distorted isotope patterns usually observed. In this work, we analyze these isotope patterns to compare the stability of nondissociative electron transfer (ETnoD) products, specifically noncovalent c/z fragment complexes, across a range of ubiquitin conformational states. Using ion mobility, we find that more extended states are more prone to fragment release. We obtain evidence that for a given charge state, populations of ubiquitin ions formed either directly by electrospray ionization or through collapse of more extended states upon charge reduction, span a similar range of collision cross-sections. Products of gas-phase collapse are, however, less stabilized towards unfolding than the native conformation, indicating that the ions retain a memory of previous conformational states. Furthermore, this collapse of charge-reduced ions is promoted if the ions are 'preheated' using collisional activation, with possible implications for the kinetics of gas-phase compaction.
Notes: [Lermyte, Frederik; Sobott, Frank] Univ Antwerp, Dept Chem, Biomol & Analyt Mass Spectrometry Grp, Antwerp, Belgium. [Lermyte, Frederik; Valkenborg, Dirk] Univ Antwerp, Ctr Prote, Antwerp, Belgium. [Lacki, Mateusz Krzysztof; Gambin, Anna] Univ Warsaw, Inst Informat, Warsaw, Poland. [Valkenborg, Dirk] Hasselt Univ, Interuniv Inst Biostat & Stat Bioinformat, Hasselt, Belgium. [Valkenborg, Dirk] Flemish Inst Technol Res VITO, Appl Bio & Mol Syst, Antwerp, Belgium. [Sobott, Frank] Univ Leeds, Astbury Ctr Struct Mol Biol, Leeds LS2 9JT, W Yorkshire, England. [Sobott, Frank] Univ Leeds, Sch Mol & Cellular Biol, Leeds LS2 9JT, W Yorkshire, England.
URI: http://hdl.handle.net/1942/23274
DOI: 10.1007/s13361-016-1444-7
ISI #: 000391433100009
ISSN: 1044-0305
Category: A1
Type: Journal Contribution
Appears in Collections: Research publications

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