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

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.

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 Creators:
Zeradjanin, Aleksandar1, Author           
Polymeros, George2, Author           
Toparli, Cigdem3, 4, Author           
Ledendecker, Marc2, 5, Author           
Hodnik, Nejc6, Author           
Erbe, Andreas3, 7, Author           
Rohwerder, Michael8, 9, Author           
La Mantia, Fabio10, 11, Author           
Affiliations:
1Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society, ou_3023874              
2Electrocatalysis, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society, ou_1863354              
3Interface Spectroscopy, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society, ou_1863358              
4Department of Metallurgical & Materials Eng., Istanbul Technical University, Istanbul, Turkey, ou_persistent22              
5Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863288              
6National Institute of Chemistry, Hajdrihova 19, Ljubljana, Slovenia, ou_persistent22              
7Department of Materials Science and Engineering, NTNU - Norwegian University of Science and Technology, 7491 Trondheim, Norway, ou_persistent22              
8Corrosion, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society, ou_2074315              
9Electrochemical Society Active Member, USA, ou_persistent22              
10Zentrum für Elektrochemie (CES), Ruhr-Universität Bochum, Universitätsstraße 150, 44801 Bochum, Germany, ou_persistent22              
11IFAM, Fachgebiet Energiespeicher- und Energiewandlersysteme, Fachbereich Produktionstechnik (FB 4), Wiener Straße 12, 28359 Bremen, ou_persistent22              

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 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.

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Language(s): eng - English
 Dates: 2020
 Publication Status: Issued
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: ISI: 000537175100049
DOI: 10.1039/d0cp01108h
 Degree: -

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Title: Physical Chemistry Chemical Physics
  Alternative Title : Phys. Chem. Chem. Phys.
Source Genre: Journal
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Publ. Info: Cambridge, England : Royal Society of Chemistry
Pages: - Volume / Issue: 22 (16) Sequence Number: - Start / End Page: 8768 - 8780 Identifier: ISSN: 1463-9076
n.a.: /journals/resource/954925272413_1