Issue 11, 2019

Interconversion of hydrated protons at the interface between liquid water and platinum

Abstract

Hydrogen transfer is the fundamental step in electrochemistry involved in water splitting and the hydrogen evolution reaction (HER). However, the nature of this process at the solid–liquid interface has been little studied at the atomic level. In this work, we use ab initio molecular dynamics (AIMD) and umbrella sampling (US), giving us an accurate description of the dynamic processes associated with the solid–liquid environment. Based on this method, the free energy barriers were calculated at the H2O/Pt(111) interface, and a multistep mechanism has been proposed. We find that proton transfer is dictated by the strength of the solid–liquid interaction and the configuration of water molecules above the reaction site. In particular, we show that the surface adsorbed cations, which are confined to the interface above the top site position, act as vessels for enhanced hydrogen transfer to and from the surface. Our results could lead to significant mechanistic consequences for the HER, water splitting and solid–liquid reactions in general.

Graphical abstract: Interconversion of hydrated protons at the interface between liquid water and platinum

Supplementary files

Article information

Article type
Paper
Submitted
10 Jan 2019
Accepted
08 Feb 2019
First published
13 Feb 2019

Phys. Chem. Chem. Phys., 2019,21, 5932-5940

Interconversion of hydrated protons at the interface between liquid water and platinum

P. S. Rice, Y. Mao, C. Guo and P. Hu, Phys. Chem. Chem. Phys., 2019, 21, 5932 DOI: 10.1039/C8CP07511E

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements