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Size effects and active state formation of cobalt oxide nanoparticles during the oxygen evolution reaction
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Journal Article
Size effects and active state formation of cobalt oxide nanoparticles during the oxygen evolution reaction
2022
Overview
Water electrolysis is a key technology to establish CO
2
-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 CoO
x
(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 Co
3+
O
6
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.
The near-surface structure of oxide electrocatalysts during the oxygen evolution reaction is key to performance but remains elusive. Here the authors use operando X-ray absorption spectroscopy to track the size-dependent catalytic activity of CoO
x
(OH)
y
nanoparticles down to 1 nm and their structural changes under reaction conditions.
Publisher
Nature Publishing Group UK,Nature Publishing Group
Subject
