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