التفاصيل البيبلوغرافية
| العنوان: |
Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction. |
| المؤلفون: |
Hsu, Chia-Shuo, Wang, Jiali, Chu, You-Chiuan, Chen, Jui-Hsien, Chien, Chia-Ying, Lin, Kuo-Hsin, Tsai, Li Duan, Chen, Hsiao-Chien, Liao, Yen-Fa, Hiraoka, Nozomu, Cheng, Yuan-Chung, Chen, Hao Ming |
| المصدر: |
Nature Communications; 8/28/2023, Vol. 14 Issue 1, p1-14, 14p |
| مصطلحات موضوعية: |
ELECTROLYTIC reduction, SURFACE charges, COPPER, ATOMIC charges, SURFACE charging, SURFACE states |
| مستخلص: |
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. Comprehensive understanding of Cu state is of high interest for CO2 electroconversion. Here, the authors reveal a dynamic low-coordinated Cu center as active site for CO2 to CO conversion and propose atomic surface charge as an indicator for evaluating CO2 electroreduction performance. [ABSTRACT FROM AUTHOR] |
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| قاعدة البيانات: |
Complementary Index |
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