文献类型：期刊文献

英文题名：Cation-Deficiency-Dependent CO2 Electroreduction over Copper-Based Ruddlesden-Popper Perovskite Oxides

作者：Zhu, Jiawei[1];Wang, Yanying[1];Zhi, Aomiao[2,3];Chen, Zitao[2,3];Shi, Lei[4];Zhang, Zhenbao[5];Zhang, Yu;Zhu, Yinlong;Qiu, Xiaoyu[8];Tian, Xuezeng[2,3];Bai, Xuedong[2,3];Zhang, Ying[1,6];Zhu, Yongfa[7,9]

机构：[1]Jiangnan Univ, Sch Chem & Mat Engn, Wuxi 214122, Jiangsu, Peoples R China;[2]Chinese Acad Sci, Beijing Natl Lab Condensed Matter Phys, Beijing 100190, Peoples R China;[3]Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China;[4]Nanjing Forestry Univ, Coll Mat Sci & Engn, Nanjing 210037, Peoples R China;[5]Jinan Univ, Dept Chem, Coll Chem & Mat Sci, Guangzhou 510632, Peoples R China;[6]East China Univ Sci & Technol, Sch Mech & Power Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[7]Monash Univ, Dept Chem Engn, Clayton, Vic 3800, Australia;[8]Nanjing Normal Univ, Sch Chem & Mat Sci, Nanjing 210023, Peoples R China;[9]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China

年份：2022

卷号：61

期号：3

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20214811219764);WOS:【SCI-EXPANDED(收录号:WOS:000720985500001)】；

基金：This research was supported by the National Natural Science Foundation of China (21902009 and 52102258), Natural Science Foundation of Jiangsu Province (BK20210447), and Start-up Funds from Jiangnan University (1045219032210010).

语种：英文

外文关键词：A-site cation deficiencies; CO2 electroreduction; CuO; perovskite hybrid; oxygen vacancies; Ruddlesden-Popper perovskite oxide

摘要：We report an effective strategy to enhance CO2 electroreduction (CER) properties of Cu-based Ruddlesden-Popper (RP) perovskite oxides by engineering their A-site cation deficiencies. With La2-xCuO4-delta (L2-xC, x=0, 0.1, 0.2, and 0.3) as proof-of-concept catalysts, we demonstrate that their CER activity and selectivity (to C2+ or CH4) show either a volcano-type or an inverted volcano-type dependence on the x values, with the extreme point at x=0.1. Among them, at -1.4 V, the L1.9C delivers the optimal activity (51.3 mA cm(-2)) and selectivity (41.5 %) for C2+, comparable to or better than those of most reported Cu-based oxides, while the L1.7C exhibits the best activity (25.1 mA cm(-2)) and selectivity (22.1 %) for CH4. Such optimized CER properties could be ascribed to the favorable merits brought by the cation-deficiency-induced oxygen vacancies and/or CuO/RP hybrids, including the facilitated adsorption/activation of key reaction species and thus the manipulated reaction pathways.