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

Fabio Dionigi (), Zhenhua Zeng (), Ilya Sinev, Thomas Merzdorf, Siddharth Deshpande, Miguel Bernal Lopez, Sebastian Kunze, Ioannis Zegkinoglou, Hannes Sarodnik, Dingxin Fan, Arno Bergmann, Jakub Drnec, Jorge Ferreira de Araujo, Manuel Gliech, Detre Teschner, Jing Zhu, Wei-Xue Li, Jeffrey Greeley, Beatriz Roldan Cuenya () and Peter Strasser ()
Additional contact information
Fabio Dionigi: Technical University Berlin
Zhenhua Zeng: Purdue University
Ilya Sinev: Ruhr-University Bochum
Thomas Merzdorf: Technical University Berlin
Siddharth Deshpande: Purdue University
Miguel Bernal Lopez: Ruhr-University Bochum
Sebastian Kunze: Ruhr-University Bochum
Ioannis Zegkinoglou: Ruhr-University Bochum
Hannes Sarodnik: Technical University Berlin
Dingxin Fan: Purdue University
Arno Bergmann: Technical University Berlin
Jakub Drnec: European Synchrotron Radiation Facility
Jorge Ferreira de Araujo: Technical University Berlin
Manuel Gliech: Technical University Berlin
Detre Teschner: Fritz-Haber-Institut der Max-Planck-Gesellschaft
Jing Zhu: School of Chemistry and Materials Science, University of Science and Technology of China
Wei-Xue Li: School of Chemistry and Materials Science, University of Science and Technology of China
Jeffrey Greeley: Purdue University
Beatriz Roldan Cuenya: Fritz-Haber-Institut der Max-Planck-Gesellschaft
Peter Strasser: Technical University Berlin

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-16237-1

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