What is the trigger for the hydrogen evolution reaction? - towards electrocatalysis beyond the Sabatier principle


Creative Commons License

Zeradjanin A. R., Polymeros G., TOPARLI Ç., Ledendecker M., Hodnik N., Erbe A., ...More

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, vol.22, no.16, pp.8768-8780, 2020 (SCI-Expanded) identifier identifier identifier

  • Publication Type: Article / Article
  • Volume: 22 Issue: 16
  • Publication Date: 2020
  • Doi Number: 10.1039/d0cp01108h
  • Journal Name: PHYSICAL CHEMISTRY CHEMICAL PHYSICS
  • Journal Indexes: Science Citation Index Expanded (SCI-EXPANDED), Scopus, Chimica, Communication Abstracts, EMBASE, INSPEC, MEDLINE
  • Page Numbers: pp.8768-8780
  • Middle East Technical University Affiliated: Yes

Abstract

The mechanism of the hydrogen evolution reaction, although intensively studied for more than a century, remains a fundamental scientific challenge. Many important questions are still open, making it elusive to establish rational principles for electrocatalyst design. In this work, a comprehensive investigation was conducted to identify which dynamic phenomena at the electrified interface are prerequisite for the formation of molecular hydrogen. In fact, what we observe as an onset of the macroscopic faradaic current originates from dynamic structural changes in the double layer, which are entropic in nature. Based on careful analysis of the activation process, an electrocatalytic descriptor is introduced, evaluated and experimentally confirmed. The catalytic activity descriptor is named as the potential of minimum entropy. The experimentally verified catalytic descriptor reveals significant potential to yield innovative insights for the design of catalytically active materials and interfaces.