Size effects and active state formation of cobalt oxide nanoparticles during the oxygen evolution reaction

Felix T. Haase, Arno Bergmann (), Travis E. Jones, Janis Timoshenko, Antonia Herzog, Hyo Sang Jeon, Clara Rettenmaier and Beatriz Roldan Cuenya ()
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Felix T. Haase: Fritz Haber Institute of the Max Planck Society
Arno Bergmann: Fritz Haber Institute of the Max Planck Society
Travis E. Jones: Fritz Haber Institute of the Max Planck Society
Janis Timoshenko: Fritz Haber Institute of the Max Planck Society
Antonia Herzog: Fritz Haber Institute of the Max Planck Society
Hyo Sang Jeon: Fritz Haber Institute of the Max Planck Society
Clara Rettenmaier: Fritz Haber Institute of the Max Planck Society
Beatriz Roldan Cuenya: Fritz Haber Institute of the Max Planck Society

Nature Energy, 2022, vol. 7, issue 8, 765-773

Abstract: Abstract Water electrolysis is a key technology to establish CO2-neutral hydrogen production. Nonetheless, the near-surface structure of electrocatalysts during the anodic oxygen evolution reaction (OER) is still largely unknown, which hampers knowledge-driven optimization. Here using operando X-ray absorption spectroscopy and density functional theory calculations, we provide quantitative near-surface structural insights into oxygen-evolving CoOx(OH)y nanoparticles by tracking their size-dependent catalytic activity down to 1 nm and their structural adaptation to OER conditions. We uncover a superior intrinsic OER activity of sub-5 nm nanoparticles and a size-dependent oxidation leading to a near-surface Co–O bond contraction during OER. We find that accumulation of oxidative charge within the surface Co3+O6 units triggers an electron redistribution and an oxyl radical as predominant surface-terminating motif. This contrasts the long-standing view of high-valent metal ions driving the OER, and thus, our advanced operando spectroscopy study provides much needed fundamental understanding of the oxygen-evolving near-surface chemistry.

Date: 2022
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DOI: 10.1038/s41560-022-01083-w

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