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Journal Article

5f Covalency Synergistically Boosting Oxygen Evolution of UCoO4 Catalyst


Hu,  Zhiwei
Zhiwei Hu, Physics of Correlated Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Lin, X., Huang, Y.-C., Hu, Z., Li, L., Zhou, J., Zhao, Q., et al. (2022). 5f Covalency Synergistically Boosting Oxygen Evolution of UCoO4 Catalyst. Journal of the American Chemical Society, 144(1), 416-423. doi:10.1021/jacs.1c10311.

Cite as: https://hdl.handle.net/21.11116/0000-0009-AFCE-B
Electronic structure modulation among multiple metal sites is key to the design of efficient catalysts. Most studies have focused on regulating 3d transition-metal active ions through other d-block metals, while few have utilized f-block metals. Herein, we report a new class of catalyst, namely, UCoO4 with alternative CoO6 and Sf-related UO6 octahedra, as a unique example of a 5f-covalent compound that exhibits enhanced electrocatalytic oxygen evolution reaction (OER) activity because of the presence of the U 5f-O 2p-Co 3d network. UCoO4 exhibits a low overpotential of 250 mV at 10 mA cm(-2), surpassing other unitary cobalt-based catalysts ever reported. X-ray absorption spectroscopy revealed that the Co(2+)ion in pristine UCoO4 was converted to high-valence Co3+/4+, while U6+ remained unchanged during the OER, indicating that only Co was the active site. Density functional theory calculations demonstrated that the OER activity of Co3+/4+ was synergistically enhanced by the covalent bonding of U6+-5f in the U 5f-O 2p-Co 3d network. This study opens new avenues for the realization of electronic structure manipulation via unique Sf involvement.