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Issue 43, 2019
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Electric field modulated redox-driven protonation and hydration energetics in energy converting enzymes

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Abstract

Biological energy conversion is catalysed by proton-coupled electron transfer (PCET) reactions that form the chemical basis of respiratory and photosynthetic enzymes. Despite recent advances in structural, biophysical, and computational experiments, the mechanistic principles of these reactions still remain elusive. Based on common functional features observed in redox enzymes, we study here generic mechanistic models for water-mediated long-range PCET reactions. We show how a redox reaction within a buried protein environment creates an electric field that induces hydration changes between the proton acceptor and donor groups, and in turn, lowers the reaction barrier and increases the thermodynamic driving forces for the water-mediated PCET process. We predict linear free energy relationships, and discuss the proposed mechanism in context of PCET in cytochrome c oxidase.

Graphical abstract: Electric field modulated redox-driven protonation and hydration energetics in energy converting enzymes

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Supplementary files

Article information


Submitted
08 Feb 2019
Accepted
01 Apr 2019
First published
08 May 2019

This article is Open Access

Chem. Commun., 2019,55, 6078-6081
Article type
Communication

Electric field modulated redox-driven protonation and hydration energetics in energy converting enzymes

P. Saura, D. M. Frey, A. P. Gamiz-Hernandez and V. R. I. Kaila, Chem. Commun., 2019, 55, 6078
DOI: 10.1039/C9CC01135H

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