| Autor: |
Chang, Chia-Jui, Lai, Yi-An, Chu, You-Chiuan, Peng, Chun-Kuo, Tan, Hui-Ying, Pao, Chih-Wen, Lin, Yan-Gu, Hung, Sung-Fu, Chen, Hsiao-Chien, Chen, Hao Ming |
| Zdroj: |
Journal of the American Chemical Society; March 2023, Vol. 145 Issue: 12 p6953-6965, 13p |
| Abstrakt: |
Copper-oxide electrocatalysts have been demonstrated to effectively perform the electrochemical CO2reduction reaction (CO2RR) toward C2+products, yet preserving the reactive high-valent CuOxhas remained elusive. Herein, we demonstrate a model system of Lewis acidic supported Cu electrocatalyst with a pulsed electroreduction method to achieve enhanced performance for C2+products, in which an optimized electrocatalyst could reach ∼76% Faradaic efficiency for C2+products (FEC2+) at ∼−0.99 V versusreversible hydrogen electrode, and the corresponding mass activity can be enhanced by ∼2 times as compared to that of conventional CuOx. In situtime-resolved X-ray absorption spectroscopy investigating the dynamic chemical/physical nature of Cu during CO2RR discloses that an activation process induced by the KOH electrolyte during pulsed electroreduction greatly enriched the Cuδ+O/Znδ+O interfaces, which further reveals that the presence of Znδ+O species under the cathodic potential could effectively serve as a Lewis acidic support for preserving the Cuδ+O species to facilitate the formation of C2+products, and the catalyst structure–property relationship of Cuδ+O/Znδ+O interfaces can be evidently realized. More importantly, we find a universality of stabilizing Cuδ+O species for various metal oxide supports and to provide a general concept of appropriate electrocatalyst–Lewis acidic support interaction for promoting C2+products. |
| Databáze: |
Supplemental Index |
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