Surface oxidation/spin state determines oxygen evolution reaction activity of cobalt-based catalysts in acidic environment

Jinzhen Huang (), Camelia Nicoleta Borca, Thomas Huthwelker, Nur Sena Yüzbasi, Dominika Baster, Mario El Kazzi, Christof W. Schneider, Thomas J. Schmidt and Emiliana Fabbri ()
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Jinzhen Huang: Paul Scherrer Institute
Camelia Nicoleta Borca: Paul Scherrer Institute
Thomas Huthwelker: Paul Scherrer Institute
Nur Sena Yüzbasi: Empa - Swiss Federal Laboratories for Materials Science and Technology
Dominika Baster: Paul Scherrer Institute
Mario El Kazzi: Paul Scherrer Institute
Christof W. Schneider: Paul Scherrer Institute
Thomas J. Schmidt: Paul Scherrer Institute
Emiliana Fabbri: Paul Scherrer Institute

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Co-based catalysts are promising candidates to replace Ir/Ru-based oxides for oxygen evolution reaction (OER) catalysis in an acidic environment. However, both the reaction mechanism and the active species under acidic conditions remain unclear. In this study, by combining surface-sensitive soft X-ray absorption spectroscopy characterization with electrochemical analysis, we discover that the acidic OER activity of Co-based catalysts are determined by their surface oxidation/spin state. Surfaces composed of only high-spin CoII are found to be not active due to their unfavorable water dissociation to form CoIII-OH species. By contrast, the presence of low-spin CoIII is essential, as it promotes surface reconstruction of Co oxides and, hence, OER catalysis. The correlation between OER activity and Co oxidation/spin state signifies a breakthrough in defining the structure-activity relationship of Co-based catalysts for acidic OER, though, interestingly, such a relationship does not hold in alkaline and neutral environments. These findings not only help to design efficient acidic OER catalysts, but also deepen the understanding of the reaction mechanism.

Date: 2024
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DOI: 10.1038/s41467-024-47409-y

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