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

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2020-04-01

Author

Zeradjanin, Aleksandar R.
Polymeros, George
Toparlı, Çiğdem
Ledendecker, Marc
Hodnik, Nejc
Erbe, Andreas
Rohwerder, Michael
La Mantia, Fabio

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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.

URI

https://hdl.handle.net/11511/93628

Journal

PHYSICAL CHEMISTRY CHEMICAL PHYSICS

DOI

https://doi.org/10.1039/d0cp01108h

Collections

Department of Metallurgical and Materials Engineering, Article

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Citation Formats

A. R. Zeradjanin et al., “What is the trigger for the hydrogen evolution reaction? - towards electrocatalysis beyond the Sabatier principle,” PHYSICAL CHEMISTRY CHEMICAL PHYSICS, vol. 22, no. 16, pp. 8768–8780, 2020, Accessed: 00, 2021. [Online]. Available: https://hdl.handle.net/11511/93628.