In situ modulating coordination fields of single-atom cobalt catalyst for enhanced oxygen reduction reaction

Meihuan Liu, Jing Zhang, Hui Su (), Yaling Jiang, Wanlin Zhou, Chenyu Yang, Shuowen Bo, Jun Pan () and Qinghua Liu ()
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Meihuan Liu: University of Science and Technology of China
Jing Zhang: University of Science and Technology of China
Hui Su: Hunan Normal University
Yaling Jiang: University of Science and Technology of China
Wanlin Zhou: University of Science and Technology of China
Chenyu Yang: University of Science and Technology of China
Shuowen Bo: University of Science and Technology of China
Jun Pan: Central South University
Qinghua Liu: University of Science and Technology of China

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Single-atom catalysts, especially those with metal−N4 moieties, hold great promise for facilitating the oxygen reduction reaction. However, the symmetrical distribution of electrons within the metal−N4 moiety results in unsatisfactory adsorption strength of intermediates, thereby limiting their performance improvements. Herein, we present atomically coordination-regulated Co single-atom catalysts that comprise a symmetry-broken Cl−Co−N4 moiety, which serves to break the symmetrical electron distribution. In situ characterizations reveal the dynamic evolution of the symmetry-broken Cl−Co−N4 moiety into a coordination-reduced Cl−Co−N2 structure, effectively optimizing the 3d electron filling of Co sites toward a reduced d-band electron occupancy (d5.8 → d5.28) under reaction conditions for a fast four-electron oxygen reduction reaction process. As a result, the coordination-regulated Co single-atom catalysts deliver a large half-potential of 0.93 V and a mass activity of 5480 A gmetal−1. Importantly, a Zn-air battery using the coordination-regulated Co single-atom catalysts as the cathode also exhibits a large power density and excellent stability.

Date: 2024
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DOI: 10.1038/s41467-024-45990-w

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