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Insights into solvent and surface charge effects on Volmer step kinetics on Pt (111)
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Insights into solvent and surface charge effects on Volmer step kinetics on Pt (111)
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Journal Article
Insights into solvent and surface charge effects on Volmer step kinetics on Pt (111)
2023
Overview
The mechanism of pH-dependent hydrogen oxidation and evolution kinetics is still a matter of significant debate. To make progress, we study the Volmer step kinetics on platinum (111) using classical molecular dynamics simulations with an embedded Anderson-Newns Hamiltonian for the redox process and constant potential electrodes. We investigate how negative electrode electrostatic potential affects Volmer step kinetics. We find that the redox solvent reorganization energy is insensitive to changes in interfacial field strength. The negatively charged surface attracts adsorbed H as well as H
+
, increasing hydrogen binding energy, but also trapping H
+
in the double layer. While more negative electrostatic potential in the double layer accelerates the oxidation charge transfer, it becomes difficult for the proton to move to the bulk. Conversely, reduction becomes more difficult because the transition state occurs farther from equilibrium solvation polarization. Our results help to clarify how the charged surface plays a role in hydrogen electrocatalysis kinetics.
Excess free charges on electrode surfaces drive changes in hydrogen electrocatalysis kinetics. Here, the authors show how redox solvent reorganization energy is insensitive to interfacial electric field strength; instead, the charged surface directly modulates proton electrochemical potential.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
