Decoupling the catalytic and degradation mechanisms of cobalt active sites during acidic water oxidation

Darcy Simondson, Marc F. Tesch (), Ioannis Spanos, Travis E. Jones, Jining Guo, Brittany V. Kerr, Manjunath Chatti, Shannon A. Bonke, Ronny Golnak, Bernt Johannessen, Jie Xiao, Douglas R. MacFarlane, Rosalie K. Hocking () and Alexandr N. Simonov ()
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Darcy Simondson: Monash University
Marc F. Tesch: Max Planck Institute for Chemical Energy Conversion
Ioannis Spanos: Max Planck Institute for Chemical Energy Conversion
Travis E. Jones: Los Alamos National Laboratory Theoretical Division
Jining Guo: Monash University
Brittany V. Kerr: Swinburne University of Technology
Manjunath Chatti: Monash University
Shannon A. Bonke: University of Cambridge
Ronny Golnak: Helmholtz-Zentrum Berlin für Materialien und Energie
Bernt Johannessen: ANSTO
Jie Xiao: Helmholtz-Zentrum Berlin für Materialien und Energie
Douglas R. MacFarlane: Monash University
Rosalie K. Hocking: Swinburne University of Technology
Alexandr N. Simonov: Monash University

Nature Energy, 2025, vol. 10, issue 8, 1013-1024

Abstract: Abstract Advancement of iridium-free catalysts for the low-pH oxygen evolution reaction (OER) is required to enable multi-gigawatt-scale proton-exchange water electrolysis. Cobalt-based materials might address this requirement, but little is known about the mechanism of operation of these OER catalysts at low pH. Here we investigate the nature and evolution of the active cobalt sites along with charge- and mass-transfer processes that support their catalytic function within a cobalt–iron–lead oxide material using in situ spectroscopic, gravimetric and electrochemical techniques. We demonstrate that corrosion of the cobalt sites and their reformation through electrooxidation of dissolved Co2+ do not affect the catalytic mechanism and are decoupled from the OER. The OER-coupled charge transfer is supported by Co(3+δ)+-oxo-species, which are structurally different from those reported for alkaline/near-neutral conditions and are formed on a relatively slow timescale of minutes. These mechanistic insights might assist in developing genuinely practical catalysts for this vital technology.

Date: 2025
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DOI: 10.1038/s41560-025-01812-x

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