https://scholars.lib.ntu.edu.tw/handle/123456789/629985
標題: | Lewis Acidic Support Boosts C-C Coupling in the Pulsed Electrochemical CO2 Reaction | 作者: | 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 HAO MING CHEN |
關鍵字: | RAY-ABSORPTION SPECTROSCOPY; CARBON-DIOXIDE; COPPER-CATALYSTS; REDUCTION; CU2O; ELECTROREDUCTION; DESIGN; STATE | 公開日期: | 29-三月-2023 | 出版社: | AMER CHEMICAL SOC | 卷: | 145 | 期: | 12 | 起(迄)頁: | 6953 | 來源出版物: | Journal of the American Chemical Society | 摘要: | Copper-oxide electrocatalysts have been demonstrated to effectively perform the electrochemical CO2 reduction reaction (CO2RR) toward C2+ products, yet preserving the reactive high-valent CuOx has 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 versus reversible hydrogen electrode, and the corresponding mass activity can be enhanced by ∼2 times as compared to that of conventional CuOx. In situ time-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. |
URI: | https://scholars.lib.ntu.edu.tw/handle/123456789/629985 | ISSN: | 0002-7863 | DOI: | 10.1021/jacs.3c00472 |
顯示於: | 化學系 |
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