Protonated Asparaginyl-Alanine Decomposition: a TCID, SORI-CID, and Computational Analysis

Journal of the American Society for Mass Spectrometry
G C BolesP B Armentrout

Abstract

Deamidation of asparagine residues, one of the fastest known post-translational modifications in proteins, plays a significant role in various biological functions and degenerative, aging diseases. Here, we present a full description of deamidation (as well as other key dissociation processes) from protonated asparaginyl-alanine, H+(AsnAla), by studying its kinetic energy-dependent threshold collision-induced dissociation (TCID) with Xe using a guided ion beam tandem mass spectrometer. Relative thresholds compare favorably with those acquired by sustained off-resonance irradiation-CID of H+(AsnAla) with Ar in a Fourier transform ion cyclotron resonance mass spectrometer. Absolute threshold energies from the TCID studies are compared to relative single point energies of major reaction species calculated at the B3LYP, B3LYP-GD3BJ, B3P86, MP2(full), and M06-2X levels of theory. Relative energies of key TSs and products allow for the characterization of the important rate-limiting steps involved in H+(AsnAla) decomposition. The influence of water solvation on key TSs is also explored computationally, where bridging the gap between gas-phase and solvated studies is an important aspect of the biological relevance of this analysis. Th...Continue Reading

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