Hydrogen Coupling on Platinum Using Artificial Neural Network Potentials and DFT

Peter S Rice, Zhi-Pan Liu, P Hu

Research output: Contribution to journalArticlepeer-review

Abstract

To date, the understanding of reactions at solid-liquid interfaces has proven challenging, mainly because of the inaccessible nature of such systems to current experimental techniques with atomic resolution. This has meant that many important features, including free energy barriers and the atomistic structure of intermediates, remain unknown. To tackle these issues, we construct and utilize a high-dimensional neural network (HDNN) potential for the simulation of hydrogen evolution at the HCl(aq)/Pt(111) interface, taking into consideration the influence of adsorbate-adsorbate, adsorbate-solvent interactions, and ion solvation explicitly. Long time scale MD simulations reveal coadsorbed H /H O on the surface. The free energy profiles for the Tafel and Heyrovsky type hydrogen coupling are extracted using umbrella sampling. It is found that the preferential mechanism can change depending on the surface coverage, highlighting the dual mechanistic nature for HER on Pt(111). Our work demonstrates the importance of controlling the solvent-substrate interactions in developing catalysts beyond Pt.
Original languageEnglish
Pages (from-to)10637-10645
JournalJournal of Physical Chemistry Letters
Volume12
Issue number43
Early online date27 Oct 2021
DOIs
Publication statusPublished - 04 Nov 2021

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