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  In-situ structure and catalytic mechanism of NiFe and CoFe layered double hydroxides during oxygen evolution

Dionigi, F., Zeng, Z., Sinev, I., Merzdorf, T., Deshpande, S., Lopez, M. B., et al. (2020). In-situ structure and catalytic mechanism of NiFe and CoFe layered double hydroxides during oxygen evolution. Nature Communications, 11: 2522. doi:10.1038/s41467-020-16237-1.

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 Creators:
Dionigi, Fabio1, Author
Zeng, Zhenhua2, Author
Sinev, Ilya3, 4, Author              
Merzdorf, Thomas1, Author
Deshpande, Siddarth2, Author
Lopez, Miguel Bernal3, 4, Author
Kunze, Sebastian3, 4, Author              
Zegkinoglou, Ioannis3, 4, Author              
Sarodnik, Hannes1, Author
Fan, Dingxin2, Author
Bergmann, Arno1, 4, Author              
Drnec, Jakub5, Author
Araujo, Jorge Ferreira De1, Author
Gilech, Manuel1, Author
Teschner, Detre6, 7, Author              
Zhu, Jing8, Author
Li, Weixue8, Author
Greeley, Jeffrey P.2, Author
Roldan Cuenya, Beatriz4, Author              
Strasser, Peter1, Author
Affiliations:
1Electrochemical Energy, Catalysis, Materials Science Laboratory, Department of Chemistry, Chemical Engineering Division, Technical University Berlin, Strasse des 17. Juni 124, Berlin 10623, Germany, ou_persistent22              
2Davidson School of Chemical Engineering, Purdue University, West Lafayette, IN 47907, United States, ou_persistent22              
3Department of Physics, Ruhr-University Bochum, Universitaetsstrasse 150, Bochum, 44801, Germany, ou_persistent22              
4Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              
5European Synchrotron Radiation Facility, ID 31 Beamline, BP 220, F-38043, Grenoble, France, ou_persistent22              
6Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
7Max Planck Institute for Chemical Energy Conversion, Max Planck Society, Mülheim an der Ruhr, DE, ou_3023867              
8CAS Excellence Center for Nanoscience, Hefei National Laboratory for Physical Sciences at Microscale, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026, China, ou_persistent22              

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 Abstract: NiFe and CoFe (MFe) layered double hydroxides (LDHs) are among the most active electrocatalysts for the alkaline oxygen evolution reaction (OER). Herein, we combine electrochemical measurements, operando X-ray scattering and absorption spectroscopy, and density functional theory (DFT) calculations to elucidate the catalytically active phase, reaction center and the OER mechanism. We provide the first direct atomic-scale evidence that, under applied anodic potentials, MFe LDHs oxidize from as-prepared α-phases to activated γ-phases. The OER-active γ-phases are characterized by about 8% contraction of the lattice spacing and switching of the intercalated ions. DFT calculations reveal that the OER proceeds via a Mars van Krevelen mechanism. The flexible electronic structure of the surface Fe sites, and their synergy with nearest-neighbor M sites through formation of O-bridged Fe-M reaction centers, stabilize OER intermediates that are unfavorable on pure M-M centers and single Fe sites, fundamentally accounting for the high catalytic activity of MFe LDHs.

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Language(s): eng - English
 Dates: 2020-03-302020-04-212020-05-20
 Publication Status: Published online
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1038/s41467-020-16237-1
 Degree: -

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Project name : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725915
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

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Title: Nature Communications
  Abbreviation : Nat. Commun.
Source Genre: Journal
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Publ. Info: London : Nature Publishing Group
Pages: 10 Volume / Issue: 11 Sequence Number: 2522 Start / End Page: - Identifier: ISSN: 2041-1723
CoNE: https://pure.mpg.de/cone/journals/resource/2041-1723