Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction
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 employ...
| Main Authors: | , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-08-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-40970-y |
| _version_ | 1797557900438142976 |
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| author | 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 Hao Ming Chen |
| author_facet | 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 Hao Ming Chen |
| author_sort | Chia-Shuo Hsu |
| collection | DOAJ |
| description | 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 (φ e) 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 φ e 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. |
| first_indexed | 2024-03-10T17:22:49Z |
| format | Article |
| id | doaj.art-ce732400a6a54c02997883b16b70152a |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-10T17:22:49Z |
| publishDate | 2023-08-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-ce732400a6a54c02997883b16b70152a2023-11-20T10:17:45ZengNature PortfolioNature Communications2041-17232023-08-0114111410.1038/s41467-023-40970-yActivating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reductionChia-Shuo Hsu0Jiali Wang1You-Chiuan Chu2Jui-Hsien Chen3Chia-Ying Chien4Kuo-Hsin Lin5Li Duan Tsai6Hsiao-Chien Chen7Yen-Fa Liao8Nozomu Hiraoka9Yuan-Chung Cheng10Hao Ming Chen11Department of Chemistry, National Taiwan UniversityDepartment of Chemistry, National Taiwan UniversityDepartment of Chemistry, National Taiwan UniversityDepartment of Chemistry, National Taiwan UniversityDepartment of Chemistry, National Taiwan UniversityMaterial and Chemical Research Laboratories, Industrial Technology Research InstituteMaterial and Chemical Research Laboratories, Industrial Technology Research InstituteCenter for Reliability Sciences and Technologies, Chang Gung UniversityNational Synchrotron Radiation Research CenterJapan Synchrotron Radiation Research InstituteDepartment of Chemistry, National Taiwan UniversityDepartment of Chemistry, National Taiwan UniversityAbstract 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 (φ e) 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 φ e 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.https://doi.org/10.1038/s41467-023-40970-y |
| spellingShingle | 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 Hao Ming Chen Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction Nature Communications |
| title | Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction |
| title_full | Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction |
| title_fullStr | Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction |
| title_full_unstemmed | Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction |
| title_short | Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction |
| title_sort | activating dynamic atomic configuration for single site electrocatalyst in electrochemical co2 reduction |
| url | https://doi.org/10.1038/s41467-023-40970-y |
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