Anionic copper complex fragmentations from enkephalins under low-energy collision-induced dissociation in an ion trap mass spectrometer

Journal of Mass Spectrometry : JMS
Anne BosséeJean-Claude Tabet

Abstract

Peptide metallation with Cu2+ was explored in the negative ESI mode using an ion trap mass spectrometer. Under these conditions, the [(M-3H) + CuII]- species formed were investigated under low-energy collision-induced dissociation conditions. MS2 experiments indicate a very different behavior of CuII metallated complexes compared with [M-H]- species. CuII induces an easy loss of CO2 and specific side-chain cleavages (by radical losses) at the C-terminal residue, as observed previously by prompt 'in source' dissociation experiments. The loss of CO2 yields an unstable carbylide that leads to further dissociations involving the migration of a proton or a hydrogen radical (through the reduction of CuII). Multistage MS3 experiments were carried out to rationalize this behavior. Fragmentation pathways are proposed in order to explain the product ions observed. The side-chain radical loss at the C-terminus was demonstrated to be a consecutive process. Finally, evidence is provided that the specific side-chain cleavages can be used for the differentiation of Leu/Ile and Gln/Lys residues when they are located at the C-terminus. The existence of a zwitterionic form in the case of the anionic YGGFK-CuII complex is proposed.

Citations

Mar 4, 2008·Journal of the American Society for Mass Spectrometry·Michel Prudent, Hubert H Girault
Dec 18, 2013·Journal of the American Society for Mass Spectrometry·Michael C ThomasGeoffrey W Nette
Aug 5, 2006·Journal of Mass Spectrometry : JMS·Mélanie LagarrigueJean-Claude Tabet
Dec 7, 2006·Journal of Mass Spectrometry : JMS·Michel BoutinJean-Claude Tabet
Jan 8, 2013·Journal of Pharmaceutical and Biomedical Analysis·Lukasz SzyrwielJustyna Brasun
Feb 17, 2018·Environmental Science and Pollution Research International·Chia-Lung ShihPao-Chi Liao
Jan 26, 2012·European Journal of Mass Spectrometry·Ivan K Chu, Julia Laskin
May 3, 2007·Mass Spectrometry Reviews·Frantisek Turecek

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