Chang, Chia-JuiChia-JuiChangLai, Yi-AnYi-AnLaiChu, You-ChiuanYou-ChiuanChuPeng, Chun-KuoChun-KuoPengTan, Hui-YingHui-YingTanPao, Chih-WenChih-WenPaoLin, Yan-GuYan-GuLinHung, Sung-FuSung-FuHungChen, Hsiao-ChienHsiao-ChienChenHAO MING CHEN2023-04-072023-04-072023-03-290002-7863https://scholars.lib.ntu.edu.tw/handle/123456789/629985Copper-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.enRAY-ABSORPTION SPECTROSCOPY; CARBON-DIOXIDE; COPPER-CATALYSTS; REDUCTION; CU2O; ELECTROREDUCTION; DESIGN; STATE[SDGs]SDG7[SDGs]SDG13journal article10.1021/jacs.3c00472369210312-s2.0-85150336189WOS:000951237100001https://api.elsevier.com/content/abstract/scopus_id/85150336189