A Tandem Strategy for Enhancing Electrochemical CO 2 Reduction Activity of Single‐Atom Cu‐S 1 N 3 Catalysts via Integration with Cu Nanoclusters
| Autor: | Fei Li, Lu-Hua Zhang, Jian Du, Datong Chen, Honghai Wang, Jiangyi Guo, Fengshou Yu, Jiayu Zhan |
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| Rok vydání: | 2021 |
| Předmět: | |
| Zdroj: | Angewandte Chemie. 133:24224-24229 |
| ISSN: | 1521-3757 0044-8249 |
| Popis: | We developed a tandem electrocatalyst for CO2 -to-CO conversion comprising the single Cu site co-coordinated with N and S anchored carbon matrix (Cu-S1 N3 ) and atomically dispersed Cu clusters (Cux ), denoted as Cu-S1 N3 /Cux . The as-prepared Cu-S1 N3 /Cux composite presents a 100 % Faradaic efficiency towards CO generation (FECO ) at -0.65 V vs. RHE and high FECO over 90 % from -0.55 to -0.75 V, outperforming the analogues with Cu-N4 (FECO only 54 % at -0.7 V) and Cu-S1 N3 (FECO 70 % at -0.7 V) configurations. The unsymmetrical Cu-S1 N3 atomic interface in the carbon basal plane possesses an optimized binding energy for the key intermediate *COOH compared with Cu-N4 site. At the same time, the adjacent Cux effectively promotes the protonation of *CO2 - by accelerating water dissociation and offering *H to the Cu-S1 N3 active sites. This work provides a tandem strategy for facilitating proton-coupled electron transfer over the atomic-level catalytic sites. |
| Databáze: | OpenAIRE |
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