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

Haase, F., Bergmann, A., Jones, T., Timoshenko, J., Herzog, A., Jeon, H., et al. (2022). Size effects and active state formation of cobalt oxide nanoparticles during the oxygen evolution reaction. Nature Energy, 7(8), 765-773. doi:10.1038/s41560-022-01083-w.

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 Creators:
Haase, Felix1, Author           
Bergmann, Arno1, Author           
Jones, Travis2, Author           
Timoshenko, Janis1, Author           
Herzog, Antonia1, Author           
Jeon, Hyosang1, Author           
Rettenmaier, Clara1, Author           
Roldan Cuenya, Beatriz1, Author           
Affiliations:
1Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              
2Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              

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 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.

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Language(s): eng - English
 Dates: 2021-07-102022-06-222022-08-08
 Publication Status: Published online
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1038/s41560-022-01083-w
 Degree: -

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Project name : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725915
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

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Title: Nature Energy
Source Genre: Journal
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Publ. Info: London : Nature Publishing Group
Pages: 9 Volume / Issue: 7 (8) Sequence Number: - Start / End Page: 765 - 773 Identifier: ISSN: 2058-7546
CoNE: https://pure.mpg.de/cone/journals/resource/2058-7546