Non-covalent ligand-oxide interaction promotes oxygen evolution

Qianbao Wu, Junwu Liang, Mengjun Xiao, Chang Long, Lei Li, Zhenhua Zeng (), Andraž Mavrič, Xia Zheng, Jing Zhu, Hai-Wei Liang, Hongfei Liu, Matjaz Valant, Wei Wang, Zhengxing Lv, Jiong Li and Chunhua Cui ()
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Qianbao Wu: University of Electronic Science and Technology of China
Junwu Liang: Yulin Normal University
Mengjun Xiao: University of Electronic Science and Technology of China
Chang Long: University of Electronic Science and Technology of China
Lei Li: University of Electronic Science and Technology of China
Zhenhua Zeng: Purdue University
Andraž Mavrič: University of Nova Gorica
Xia Zheng: University of Electronic Science and Technology of China
Jing Zhu: University of Science and Technology of China
Hai-Wei Liang: University of Science and Technology of China
Hongfei Liu: University of Electronic Science and Technology of China
Matjaz Valant: University of Nova Gorica
Wei Wang: University of Electronic Science and Technology of China
Zhengxing Lv: Shanghai Advanced Research Institute, Chinese Academy of Sciences
Jiong Li: Shanghai Advanced Research Institute, Chinese Academy of Sciences
Chunhua Cui: University of Electronic Science and Technology of China

Nature Communications, 2023, vol. 14, issue 1, 1-12

Abstract: Abstract Strategies to generate high-valence metal species capable of oxidizing water often employ composition and coordination tuning of oxide-based catalysts, where strong covalent interactions with metal sites are crucial. However, it remains unexplored whether a relatively weak “non-bonding” interaction between ligands and oxides can mediate the electronic states of metal sites in oxides. Here we present an unusual non-covalent phenanthroline-CoO2 interaction that substantially elevates the population of Co4+ sites for improved water oxidation. We find that phenanthroline only coordinates with Co2+ forming soluble Co(phenanthroline)2(OH)2 complex in alkaline electrolytes, which can be deposited as amorphous CoOxHy film containing non-bonding phenanthroline upon oxidation of Co2+ to Co3+/4+. This in situ deposited catalyst demonstrates a low overpotential of 216 mV at 10 mA cm−2 and sustainable activity over 1600 h with Faradaic efficiency above 97%. Density functional theory calculations reveal that the presence of phenanthroline can stabilize CoO2 through the non-covalent interaction and generate polaron-like electronic states at the Co-Co center.

Date: 2023
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DOI: 10.1038/s41467-023-36718-3

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