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Conformationally driven gas-phase H/D exchange of dinucleotide negative ions
Authors:Dorothée Balbeur  Dominique Dehareng  Edwin De Pauw
Affiliation:Laboratory of Mass Spectrometry, University of Liège, Liège, Belgium. dbalbeur@ulg.ac.be
Abstract:Gas-phase hydrogen/deuterium exchange of six deprotonated dinucleotides with CD(3)OD was performed in the second hexapole of a Fourier transform ion-cyclotron resonance (FTICR) mass spectrometer. To complete these experiments, dynamic simulations were carried out to investigate the different conformations adopted by the dinucleotides. In the experimental conditions and in integrating the experimental and theoretical results, H/D exchange was shown to be controlled by hydrogen accessibility and not by the chemical nature of the heteroatom bearing the exchangeable hydrogen. A model including simultaneous H/D exchanges at the experimental time scale was used to reproduce the dinucleotide H/D exchange kinetic plots. The relay mechanism was not relevant for dinucleotides. This allowed the H/D exchange rates to be directly linked to conformations.
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