Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction

Chia-Shuo Hsu, Jiali Wang, You-Chiuan Chu, Jui-Hsien Chen, Chia-Ying Chien, Kuo-Hsin Lin, Li Duan Tsai, Hsiao-Chien Chen, Yen-Fa Liao, Nozomu Hiraoka, Yuan-Chung Cheng () and Hao Ming Chen ()
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Chia-Shuo Hsu: National Taiwan University
Jiali Wang: National Taiwan University
You-Chiuan Chu: National Taiwan University
Jui-Hsien Chen: National Taiwan University
Chia-Ying Chien: National Taiwan University
Kuo-Hsin Lin: Industrial Technology Research Institute
Li Duan Tsai: Industrial Technology Research Institute
Hsiao-Chien Chen: Chang Gung University
Yen-Fa Liao: National Synchrotron Radiation Research Center
Nozomu Hiraoka: Japan Synchrotron Radiation Research Institute
Yuan-Chung Cheng: National Taiwan University
Hao Ming Chen: National Taiwan University

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

Abstract: Abstract One challenge for realizing high-efficiency electrocatalysts for CO2 electroreduction is lacking in comprehensive understanding of potential-driven chemical state and dynamic atomic-configuration evolutions. Herein, by using a complementary combination of in situ/operando methods and employing copper single-atom electrocatalyst as a model system, we provide evidence on how the complex interplay among dynamic atomic-configuration, chemical state change and surface coulombic charging determines the resulting product profiles. We further demonstrate an informative indicator of atomic surface charge (φe) for evaluating the CO2RR performance, and validate potential-driven dynamic low-coordinated Cu centers for performing significantly high selectivity and activity toward CO product over the well-known four N-coordinated counterparts. It indicates that the structural reconstruction only involved the dynamic breaking of Cu–N bond is partially reversible, whereas Cu–Cu bond formation is clearly irreversible. For all single-atom electrocatalysts (Cu, Fe and Co), the φe value for efficient CO production has been revealed closely correlated with the configuration transformation to generate dynamic low-coordinated configuration. A universal explication can be concluded that the dynamic low-coordinated configuration is the active form to efficiently catalyze CO2-to-CO conversion.

Date: 2023
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DOI: 10.1038/s41467-023-40970-y

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