Dynamic Metal-Ligand Coordination Boosts CO2 Electroreduction
The interfacial structure of heterogeneous catalysts determines the reaction rate by adjusting the adsorption behavior of reaction intermediates. Unfortunately, the catalytic performance of conventionally static active sites has always been limited by the adsorbate linear scaling relationship. Herein, we develop a triazole-modified Ag crystal (Ag crystal-triazole) with dynamic and reversible interfacial structures to break such a relationship for boosting the catalytic activity of CO2 electroreduction into CO. On the basis of surface science measurements and theoretical calculations, we demonstrated the dynamic transformation between adsorbed triazole and adsorbed triazolyl on the Ag(111) facet induced by metal-ligand conjugation. During CO2 electroreduction, Ag crystal-triazole with the dynamically reversible transformation of ligands exhibited a faradic efficiency for CO of 98% with a partial current density for CO as high as -802.5 mA cm-2. The dynamic metal-ligand coordination not only reduced the activation barriers of CO2 protonation but also switched the rate-determining step from CO2 protonation to the breakage of C-OH in the adsorbed COOH intermediate. This work provided an atomic-level insight into the interfacial engineering of the heterogeneous catalysts toward highly efficient CO2 electroreduction.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2023 |
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| Erschienen: |
2023 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:145 |
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| Enthalten in: |
Journal of the American Chemical Society - 145(2023), 27 vom: 12. Juli, Seite 14903-14911 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Kong, Xiangdong [VerfasserIn] |
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| Links: |
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| Anmerkungen: |
Date Completed 12.07.2023 Date Revised 18.07.2023 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1021/jacs.3c04143 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM358139376 |
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| 500 | |a Date Revised 18.07.2023 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a The interfacial structure of heterogeneous catalysts determines the reaction rate by adjusting the adsorption behavior of reaction intermediates. Unfortunately, the catalytic performance of conventionally static active sites has always been limited by the adsorbate linear scaling relationship. Herein, we develop a triazole-modified Ag crystal (Ag crystal-triazole) with dynamic and reversible interfacial structures to break such a relationship for boosting the catalytic activity of CO2 electroreduction into CO. On the basis of surface science measurements and theoretical calculations, we demonstrated the dynamic transformation between adsorbed triazole and adsorbed triazolyl on the Ag(111) facet induced by metal-ligand conjugation. During CO2 electroreduction, Ag crystal-triazole with the dynamically reversible transformation of ligands exhibited a faradic efficiency for CO of 98% with a partial current density for CO as high as -802.5 mA cm-2. The dynamic metal-ligand coordination not only reduced the activation barriers of CO2 protonation but also switched the rate-determining step from CO2 protonation to the breakage of C-OH in the adsorbed COOH intermediate. This work provided an atomic-level insight into the interfacial engineering of the heterogeneous catalysts toward highly efficient CO2 electroreduction | ||
| 650 | 4 | |a Journal Article | |
| 700 | 1 | |a Zhao, Jiankang |e verfasserin |4 aut | |
| 700 | 1 | |a Xu, Zifan |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Zhengya |e verfasserin |4 aut | |
| 700 | 1 | |a Wu, Yingying |e verfasserin |4 aut | |
| 700 | 1 | |a Shi, Yaohui |e verfasserin |4 aut | |
| 700 | 1 | |a Li, Hongliang |e verfasserin |4 aut | |
| 700 | 1 | |a Ma, Chuanxu |e verfasserin |4 aut | |
| 700 | 1 | |a Zeng, Jie |e verfasserin |4 aut | |
| 700 | 1 | |a Geng, Zhigang |e verfasserin |4 aut | |
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