Theory of the transition from sequential to concerted electrochemical proton–electron transfer

Abstract

A theory for the calculation of potential energy surfaces of electrochemical proton-coupled electron transfer is considered and parameterized on the basis of thermodynamic relations. The paper discusses the qualitatively different potential energy surfaces predicted by the theory, and their relation to the existence of sequential and concerted proton-electron transfer pathways. The concomitant activation energies for sequential and concerted PET are calculated. The applied overpotential may change the qualitative shape of the PES and therefore the mechanism of the proton-coupled electron transfer reaction.

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