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  Operando Phonon Studies of the Protonation Mechanism in Highly Active Hydrogen Evolution Reaction Pentlandite Catalysts

Zegkinoglou, I., Zendegani, A., Sinev, I., Kunze, S., Mistry, H., Jeon, H. S., et al. (2017). Operando Phonon Studies of the Protonation Mechanism in Highly Active Hydrogen Evolution Reaction Pentlandite Catalysts. Journal of the American Chemical Society, 139(41), 14360-14363. doi:10.1021/jacs.7b07902.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002E-2985-2 Version Permalink: http://hdl.handle.net/11858/00-001M-0000-002E-2A20-B
Genre: Journal Article

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 Creators:
Zegkinoglou, Ioannis1, Author              
Zendegani, Ali2, Author              
Sinev, Ilya3, Author              
Kunze, Sebastian3, Author              
Mistry, Hemma3, 4, Author              
Jeon, Hyo Sang3, Author              
Zhao, Jiyong5, Author              
Hu, Michael Y.5, Author              
Alp, E. Ercan5, Author              
Piontek, Stefan6, Author              
Smialkowski, Mathias6, Author              
Apfel, Ulf-Peter6, Author              
Körmann, Fritz2, Author              
Neugebauer, Jörg7, Author              
Hickel, Tilmann2, Author              
Roldan Cuenya, Beatriz3, 8, Author              
Affiliations:
1Department of Physics, Ruhr-University Bochum, Germany, persistent22              
2Computational Phase Studies, Computational Materials Design, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society, ou_1863341              
3Department of Physics, Ruhr-University Bochum, 44780 Bochum, Germany, persistent22              
4Department of Physics, University of Central Florida, Orlando, Florida 32816, USA, persistent22              
5Advanced Photon Source, Argonne National Laboratory, Lemont, Illinois 60439, USA, persistent22              
6Inorganic Chemistry I, Ruhr-University Bochum, 44780 Bochum, Germany, persistent22              
7Computational Materials Design, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society, ou_1863337              
8Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              

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 Abstract: Synthetic pentlandite (Fe4.5Ni4.5S8) is a promising.electrocatalyst for hydrogen evolution, demonstrating high current densities, low overpotential and remarkable stability in bulk form. The depletion of sulfur from the surface of this catalyst during the electrochemical reaction has been proposed to be beneficial for its catalytic performance, but the role of sulfur vacancies and the mechanism determining the reaction kinetics are still unknown. We have performed electrochemical operando studies of the vibrational dynamics of pentlandite under hydrogen evolution reaction conditions using 57Fe nuclear resonant inelastic Xray scattering. Comparing the measured partial (Feprojected) vibrational density of states with density functional theory calculations, we have demonstrated that hydrogen atoms preferentially occupy substitutional positions replacing pre-existing sulfur vacancies. Once all vacancies are filled, the protonation proceeds interstitially, which slows down the reaction. Our results highlight the beneficial role of sulfur vacancies in the electrocatalytic performance of pentlandite and give insights into the hydrogen adsorption mechanism during the reaction.

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Language(s): eng - English
 Dates: 2017-07-272017-09-222017-10-18
 Publication Status: Published in print
 Pages: 4
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1021/jacs.7b07902
 Degree: -

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Title: Journal of the American Chemical Society
  Other : J. Am. Chem. Soc.
  Abbreviation : JACS
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: 4 Volume / Issue: 139 (41) Sequence Number: - Start / End Page: 14360 - 14363 Identifier: ISSN: 0002-7863
CoNE: /journals/resource/954925376870