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

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Sinev,  Ilya
Department of Physics, Ruhr-University Bochum, 44780 Bochum, Germany;
Interface Science, Fritz Haber Institute, Max Planck Society;

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Kunze,  Sebastian
Department of Physics, Ruhr-University Bochum, 44780 Bochum, Germany;
Interface Science, Fritz Haber Institute, Max Planck Society;

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Bergmann,  Arno
Interface Science, Fritz Haber Institute, Max Planck Society;
Department of Chemistry, Chemical Engineering Division, Technical University of Berlin;

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Teschner,  Detre
Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society;

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Strasser,  Peter
Department of Chemistry, Technical University Berlin, Straße des 17., Berlin, Germany ;
Physical Chemistry, Fritz Haber Institute, Max Planck Society;
Ertl Center for Electrochemistry and Catalysis, Gwangju Institute of Science and Technology, Gwangju 500-712, South Korea;

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Citation

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(1): 2522. doi:10.1038/s41467-020-16237-1.


Cite as: http://hdl.handle.net/21.11116/0000-0007-A482-C
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 alpha -phases to activated gamma -phases. The OER-active gamma -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. NiFe and CoFe layered double hydroxides are among the most active electrocatalysts for the alkaline oxygen evolution reaction. Here, by combining operando experiments and rigorous DFT calculations, the authors unravel their active phase, the reaction center and the catalytic mechanism.