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The concerted proton-electron transfer mechanism of proton migration in the electrochemical interface.

ABSTRACT: The proton migration in the electrochemical interface is a fundamental electrochemical processes in proton involved reactions. We find fractional electron transfer, which is inversely proportional to the distance between the proton and electrode, during the proton migration under constant potential. The electrical energy carried by the transferred charge facilitates the proton to overcome the chemical barrier in the migration pathway, which is accounting for more than half electrical energy in the proton involved reactions. Consequently, less charge transfer and energy exchange take place in the reduction process. Therefore, the proton migration in the electrochemical interface is an essential component of the electrochemical reaction in terms of electron transfer and energy conversation, and are worthy of more attention in the rational design and optimization of electrochemical systems.

SUBMITTER: Gao G

PROVIDER: S-EPMC10661362 | biostudies-literature | 2023 Nov

REPOSITORIES: biostudies-literature

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The concerted proton-electron transfer mechanism of proton migration in the electrochemical interface.

Gao Guoping G Wang Lin-Wang LW

iScience 20231029 11

The proton migration in the electrochemical interface is a fundamental electrochemical processes in proton involved reactions. We find fractional electron transfer, which is inversely proportional to the distance between the proton and electrode, during the proton migration under constant potential. The electrical energy carried by the transferred charge facilitates the proton to overcome the chemical barrier in the migration pathway, which is accounting for more than half electrical energy in t ...[more]

PMID: 38026153

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Project description:The coupling between electrons and protons and the long-range transport of protons play important roles throughout biology. Biomimetic systems derived from benzimidazole-phenol (BIP) constructs have been designed to undergo proton-coupled electron transfer (PCET) upon electrochemical or photochemical oxidation. Moreover, these systems can transport protons along hydrogen-bonded networks or proton wires through multiproton PCET. Herein, the nonequilibrium dynamics of both single and double proton transfer in BIP molecules initiated by oxidation are investigated with first-principles molecular dynamics simulations. Although these processes are concerted in that no thermodynamically stable intermediate is observed, the simulations predict that they are predominantly asynchronous on the ultrafast time scale. For both systems, the first proton transfer typically occurs ∼100 fs after electron transfer. For the double proton transfer system, typically the second proton transfer occurs hundreds of femtoseconds after the initial proton transfer. A machine learning algorithm was used to identify the key molecular vibrational modes essential for proton transfer: a slow, in-plane bending mode that dominates the overall inner-sphere reorganization, the proton donor-acceptor motion that leads to vibrational coherence, and the faster donor-hydrogen stretching mode. The asynchronous double proton transfer mechanism can be understood in terms of a significant mode corresponding to the two anticorrelated proton donor-acceptor motions, typically decreasing only one donor-acceptor distance at a time. Although these PCET processes appear concerted on the time scale of typical electrochemical experiments, attaching these BIP constructs to photosensitizers may enable the detection of the asynchronicity of the electron and multiple proton transfers with ultrafast two-dimensional spectroscopy. Understanding the fundamental PCET mechanisms at this level will guide the design of PCET systems for catalysis and energy conversion processes.

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The concerted proton-electron transfer mechanism of proton migration in the electrochemical interface.

Publications

The concerted proton-electron transfer mechanism of proton migration in the electrochemical interface.

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