Constructing asymmetric double-atomic sites for synergistic catalysis of electrochemical CO2 reduction

Jiqing Jiao (), Qing Yuan, Meijie Tan, Xiaoqian Han, Mingbin Gao, Chao Zhang, Xuan Yang (), Zhaolin Shi, Yanbin Ma, Hai Xiao, Jiangwei Zhang () and Tongbu Lu ()
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Jiqing Jiao: Tianjin University of Technology
Qing Yuan: Huazhong University of Science and Technology
Meijie Tan: Tianjin University of Technology
Xiaoqian Han: Tianjin University of Technology
Mingbin Gao: Chinese Academy of Sciences
Chao Zhang: Tianjin University of Technology
Xuan Yang: Huazhong University of Science and Technology
Zhaolin Shi: Tianjin University of Technology
Yanbin Ma: Tianjin University of Technology
Hai Xiao: Tsinghua University
Jiangwei Zhang: Inner Mongolia University
Tongbu Lu: Tianjin University of Technology

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

Abstract: Abstract Elucidating the synergistic catalytic mechanism between multiple active centers is of great significance for heterogeneous catalysis; however, finding the corresponding experimental evidence remains challenging owing to the complexity of catalyst structures and interface environment. Here we construct an asymmetric TeN2–CuN3 double-atomic site catalyst, which is analyzed via full-range synchrotron pair distribution function. In electrochemical CO2 reduction, the catalyst features a synergistic mechanism with the double-atomic site activating two key molecules: operando spectroscopy confirms that the Te center activates CO2, and the Cu center helps to dissociate H2O. The experimental and theoretical results reveal that the TeN2–CuN3 could cooperatively lower the energy barriers for the rate-determining step, promoting proton transfer kinetics. Therefore, the TeN2–CuN3 displays a broad potential range with high CO selectivity, improved kinetics and good stability. This work presents synthesis and characterization strategies for double-atomic site catalysts, and experimentally unveils the underpinning mechanism of synergistic catalysis.

Date: 2023
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DOI: 10.1038/s41467-023-41863-w

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