Voltage- and time-dependent valence state transition in cobalt oxide catalysts during the oxygen evolution reaction

Jing Zhou, Linjuan Zhang (), Yu-Cheng Huang, Chung-Li Dong, Hong-Ji Lin, Chien-Te Chen, L. H. Tjeng and Zhiwei Hu ()
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Jing Zhou: Chinese Academy of Sciences
Linjuan Zhang: Chinese Academy of Sciences
Yu-Cheng Huang: Tamkang University
Chung-Li Dong: Tamkang University
Hong-Ji Lin: National Synchrotron Radiation Research Center
Chien-Te Chen: National Synchrotron Radiation Research Center
L. H. Tjeng: Max Planck Institute for Chemical Physics of Solids
Zhiwei Hu: Max Planck Institute for Chemical Physics of Solids

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: Abstract The ability to determine the electronic structure of catalysts during electrochemical reactions is highly important for identification of the active sites and the reaction mechanism. Here we successfully applied soft X-ray spectroscopy to follow in operando the valence and spin state of the Co ions in Li2Co2O4 under oxygen evolution reaction (OER) conditions. We have observed that a substantial fraction of the Co ions undergo a voltage-dependent and time-dependent valence state transition from Co3+ to Co4+ accompanied by spontaneous delithiation, whereas the edge-shared Co–O network and spin state of the Co ions remain unchanged. Density functional theory calculations indicate that the highly oxidized Co4+ site, rather than the Co3+ site or the oxygen vacancy site, is mainly responsible for the high OER activity.

Date: 2020
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DOI: 10.1038/s41467-020-15925-2

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