We report some preliminary results of our computational studies on the proton transport mechanism associated with catalytic reduction of protons and oxidation of H2 in [FeFe] hydrogenese enzymes. We have modeled a number of protonated states in the proposed reaction path that has recently been confirmed as the most probable route for proton delivery to the active site, and find that the network of stable hydrogen bonding between the residues considered to be part of the Grotthuss mechanism rearranges due to the protonation. We also quantified the reaction energies and find proton transfer via this pathway to be thermodynamically favorable. Our current work involves more detailed analysis of the dynamics in this system, including exploration of the free energy surface and estimates of barriers to reaction.

Theoretical study of different protonation states in proton transport model In [FeFe] hydrogenase

243rd National Meeting (2012)

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