Regulating Co–O covalency to manipulate mechanistic transformation for 
enhancing activity/durability in acidic water oxidation

Zhang, Jiachen; Chen, Guangbo; Sun, Dongmei; Tang, Yawen; Xing, Wei; Sun, Hanjun; Feng, Xinliang

doi:10.1039/D4SC05547K

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Regulating Co–O covalency to manipulate mechanistic transformation for enhancing activity/durability in acidic water oxidation

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Feng, Xinliang
Department of Synthetic Materials and Functional Devices (SMFD), Max Planck Institute of Microstructure Physics, Max Planck Society;

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https://doi.org/10.1039/D4SC05547K
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Citation

Zhang, J., Chen, G., Sun, D., Tang, Y., Xing, W., Sun, H., et al. (2024). Regulating Co–O covalency to manipulate mechanistic transformation for enhancing activity/durability in acidic water oxidation. Chemical Science. doi:10.1039/D4SC05547K.

Cite as: https://hdl.handle.net/21.11116/0000-000F-F3D5-E

Abstract

Developing earth-abundant electrocatalysts with high activity and durability for acidic oxygen evolution reaction is essential for H₂ production, yet it remains greatly challenging. Here, guided by theoretical calculations, the challenge of overcoming the balance between catalytic activity and dynamic durability for acidic OER in Co₃O₄ was effectively addressed via the preferential substitution of Ru for the Co²⁺ (Td) site of Co₃O₄. In situ characterization and DFT calculations show that the enhanced Co–O covalency after the introduction of Ru SAs facilitates the generation of OH* species and mitigates the unstable structure transformation via direct O–O coupling. The designed Ru SAs-CoO_x catalyst (5.16 wt% Ru) exhibits enhanced OER activity (188 mV overpotential at 10 mA cm⁻²) and durability, outperforming most reported Co₃O₄-based and Ru-based electrocatalysts in acidic media.