Determination of peptide topology through time-resolved double-resonance under electron capture dissociation conditions

Analytical Chemistry
Marie Pérot-TaillandierCarlos Afonso

Abstract

Characterizing the conformation of biomolecules by mass spectrometry still represents a challenge. With their knotted structure involving a N-terminal macrolactam ring where the C-terminal tail of the peptide is threaded and sterically trapped, lasso peptides constitute an attractive model for developing methods for characterizing gas-phase conformation, through comparison with their unknotted topoisomers. Here, the kinetics of electron capture dissociation (ECD) of a lasso peptide, capistruin, was investigated by electrospray ionization-Fourier transform ion cyclotron resonance mass spectrometry and compared to that of its branched-cyclic topoisomer, lactam-capistruin. Both peptides produced rather similar ECD spectra but showed different extent of H(•) transfer from c(i)' to z(j)(•) ions. Time-resolved double-resonance experiments under ECD conditions were performed to measure the formation rate constants of typical product ions. Such experiments showed that certain product ions, in particular those related to H(•) transfer, proceeded through long-lived complexes for capistruin, while fast dissociation processes predominated for lactam-capistruin. The formation rate constants of specific ECD product ions enabled a clear diffe...Continue Reading

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Citations

Jun 1, 2013·Journal of the American Society for Mass Spectrometry·Chafia BennaceurJean-Claude Tabet
Nov 28, 2012·Chemistry : a European Journal·Marie Pérot-TaillandierCarlos Afonso
Jul 7, 2015·Rapid Communications in Mass Spectrometry : RCM·Kevin Jeanne Dit FouqueFabien Chirot
Apr 15, 2015·Journal of the American Society for Mass Spectrometry·Moritz Schennach, Kathrin Breuker
Jun 30, 2018·Organic & Biomolecular Chemistry·Helena Martin-Gómez, Judit Tulla-Puche
Feb 7, 2018·The Analyst·K Jeanne Dit FouqueC Afonso
Jun 10, 2021·Analytical and Bioanalytical Chemistry·Kevin Jeanne Dit FouqueFrancisco Fernandez-Lima
Dec 17, 2014·Analytical Chemistry·Kevin Jeanne Dit FouqueHélène Lavanant
Oct 27, 2021·Analytical Methods : Advancing Methods and Applications·K Jeanne Dit FouqueF Fernandez-Lima

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