Reversible amorphization and the catalytically active state of crystalline Co3O4 during oxygen evolution

Arno Bergmann (), Elias Martinez-Moreno, Detre Teschner, Petko Chernev, Manuel Gliech, Jorge Ferreira de Araújo, Tobias Reier, Holger Dau () and Peter Strasser ()
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Arno Bergmann: Electrochemical Energy, Catalysis and Materials Science Laboratory, Technische Universität Berlin
Elias Martinez-Moreno: Freie Universität Berlin
Detre Teschner: Fritz-Haber-Institute of the Max-Planck-Society
Petko Chernev: Freie Universität Berlin
Manuel Gliech: Electrochemical Energy, Catalysis and Materials Science Laboratory, Technische Universität Berlin
Jorge Ferreira de Araújo: Electrochemical Energy, Catalysis and Materials Science Laboratory, Technische Universität Berlin
Tobias Reier: Electrochemical Energy, Catalysis and Materials Science Laboratory, Technische Universität Berlin
Holger Dau: Freie Universität Berlin
Peter Strasser: Electrochemical Energy, Catalysis and Materials Science Laboratory, Technische Universität Berlin

Nature Communications, 2015, vol. 6, issue 1, 1-9

Abstract: Abstract Water splitting catalysed by earth-abundant materials is pivotal for global-scale production of non-fossil fuels, yet our understanding of the active catalyst structure and reactivity is still insufficient. Here we report on the structurally reversible evolution of crystalline Co3O4 electrocatalysts during oxygen evolution reaction identified using advanced in situ X-ray techniques. At electrode potentials facilitating oxygen evolution, a sub-nanometre shell of the Co3O4 is transformed into an X-ray amorphous CoOx(OH)y which comprises di-μ-oxo-bridged Co3+/4+ ions. Unlike irreversible amorphizations, here, the formation of the catalytically-active layer is reversed by re-crystallization upon return to non-catalytic electrode conditions. The Co3O4 material thus combines the stability advantages of a controlled, stable crystalline material with high catalytic activity, thanks to the structural flexibility of its active amorphous oxides. We propose that crystalline oxides may be tailored for generating reactive amorphous surface layers at catalytic potentials, just to return to their stable crystalline state under rest conditions.

Date: 2015
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DOI: 10.1038/ncomms9625

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