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

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Zeradjanin,  Aleksandar
Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society;

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Polymeros,  George
Electrocatalysis, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Toparli,  Cigdem
Interface Spectroscopy, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;
Department of Metallurgical & Materials Eng., Istanbul Technical University, Istanbul, Turkey;

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Ledendecker,  Marc
Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society;
Electrocatalysis, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Erbe,  Andreas
Interface Spectroscopy, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;
Department of Materials Science and Engineering, NTNU - Norwegian University of Science and Technology, 7491 Trondheim, Norway;

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Rohwerder,  Michael
Corrosion, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;
Electrochemical Society Active Member, USA;

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Citation

Zeradjanin, A., Polymeros, G., Toparli, C., Ledendecker, M., Hodnik, N., Erbe, A., et al. (2020). What is the trigger for the hydrogen evolution reaction? - towards electrocatalysis beyond the Sabatier principle. Physical Chemistry Chemical Physics, 22(16), 8768-8780. doi:10.1039/d0cp01108h.


Cite as: http://hdl.handle.net/21.11116/0000-0007-D51F-7
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.