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

Dionigi, Fabio; Zeng, Zhenhua; Sinev, Ilya; Merzdorf, Thomas; Deshpande, Siddarth; Lopez, Miguel Bernal; Kunze, Sebastian; Zegkinoglou, Ioannis; Sarodnik, Hannes; Fan, Dingxin; Bergmann, Arno; Drnec, Jakub; Araujo, Jorge Ferreira De; Gilech, Manuel; Teschner, Detre; Zhu, Jing; Li, Weixue; Greeley, Jeffrey P.; Roldan Cuenya, Beatriz; Strasser, Peter; Strasser, Peter

doi:10.1038/s41467-020-16237-1

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

MPG-Autoren

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

Lopez, Miguel Bernal
Department of Physics, Ruhr-University Bochum;
Interface Science, Fritz Haber Institute, Max Planck Society;

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

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Zegkinoglou, Ioannis
Department of Physics, Ruhr-University Bochum;
Interface Science, Fritz Haber Institute, Max Planck Society;

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

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Teschner, Detre
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Max Planck Institute for Chemical Energy Conversion, Max Planck Society;

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Roldan Cuenya, Beatriz
Interface Science, Fritz Haber Institute, Max Planck Society;

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Zitation

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.

Zitierlink: https://hdl.handle.net/21.11116/0000-0006-80FC-D

Zusammenfassung

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.