Reaction pathway of oxygen evolution on Pt(111) revealed through constant Fermi level molecular dynamics

TL;DR

This study uses constant Fermi level molecular dynamics to reveal the oxygen evolution pathway on Pt(111), showing adsorbate arrangements, reaction intermediates, and overpotential reduction, providing insights into catalytic mechanisms.

Contribution

It introduces a novel application of constant Fermi level molecular dynamics to explore catalytic reaction pathways at the atomic level.

Findings

Adsorbates form a hexagonal lattice with irregular alternation.

Oxygen evolution proceeds via a hydrogen peroxide intermediate.

Overpotential is reduced by 0.2 eV compared to previous mechanisms.

Abstract

The pathway of the oxygen evolution reaction at the Pt(111)/water interface is disclosed through constant Fermi level molecular dynamics. Upon the application of a positive bias potential H 2 O ads and OH ads adsorbates are found to arrange in a hexagonal lattice with an irregular alternation. Increasing further the electrode potential then induces the oxygen evolution reaction, which is found to proceed through a hydrogen peroxide intermediate. Calculation of the associated overpotential shows a reduction of 0.2 eV compared to the associative mechanism. This result highlights the forcefullness of the applied scheme in exploring catalytic reactions in an unbiased way.