文献类型：期刊文献

英文题名：Promoting CO2 Electroreduction Over Nano-Socketed Cu/Perovskite Heterostructures via A-Site-Valence-Controlled Oxygen Vacancies

作者：Chen, Mingfa[1];Xu, Yunze[2,3];Zhang, Yu[2,3,7];Zhang, Zhenbao[4];Li, Xueyan[2,5];Wang, Qi[2,3];Huang, Minghua[5];Fang, Wei[6];Jiang, Heqing[2,3];Zhu, Yongfa[8];Zhu, Jiawei[1,2,3]

机构：[1]Jiangnan Univ, Sch Chem & Mat Engn, Key Lab Synthet & Biol Colloids, Minist Educ, Wuxi 214122, Peoples R China;[2]Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, Qingdao 266101, Peoples R China;[3]Shandong Energy Inst, Qingdao 266101, Peoples R China;[4]Linyi Univ, Sch Chem & Chem Engn, Linyi 276005, Peoples R China;[5]Ocean Univ China, Sch Mat Sci & Engn, Qingdao 266100, Peoples R China;[6]Ningbo Univ, Sch Mat Sci & Chem Engn, Ningbo 315211, Peoples R China;[7]East China Univ Sci & Technol, Sch Mech & Power Engn, Shanghai 200237, Peoples R China;[8]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China

年份：2024

卷号：20

期号：32

外文期刊名：SMALL

收录：;EI(收录号：20241115746612);WOS:【SCI-EXPANDED(收录号:WOS:001184386100001)】；

基金：M.C., Y.X., and Y.Z. contributed equally to this work. This research was supported by the National Natural Science Foundation of China (52102258), the Taishan Scholars Program (tsqn202306309), the Natural Science Foundation of Shandong Province (ZR2023YQ012), the Natural Science Foundation of Jiangsu Province (BK20210447), and the Special Fund Project of Jiangsu Province for Scientific and Technological Innovation in Carbon Peaking and Carbon Neutrality (BK20220023).

语种：英文

外文关键词：C2+ production; CO2 electroreduction; Cu/perovskite heterostructure; Nano-socketed Cu; Oxygen vacancy

摘要：Despite the intriguing potential, nano-socketed Cu/perovskite heterostructures for CO2 electroreduction (CO2RR) are still in their infancy and rational optimization of their CO2RR properties is lacking. Here, an effective strategy is reported to promote CO2-to-C2+ conversion over nano-socketed Cu/perovskite heterostructures by A-site-valence-controlled oxygen vacancies. For the proof-of-concept catalysts of Cu/La0.3-xSr0.6+xTiO3-delta (x from 0 to 0.3), their oxygen vacancy concentrations increase controllably with the decreased A-site valences (or the increased x values). In flow cells, their activity and selectivity for C2+ present positive correlations with the oxygen vacancy concentrations. Among them, the Cu/Sr0.9TiO3-delta with most oxygen vacancies shows the optimal activity and selectivity for C2+. And relative to the Cu/La0.3Sr0.6TiO3-delta with minimum oxygen vacancies, the Cu/Sr0.9TiO3-delta exhibits marked improvements (up to 2.4 folds) in activity and selectivity for C2+. The experiments and theoretical calculations suggest that the optimized performance can be attributed to the merits provided by oxygen vacancies, including the accelerated charge transfer, enhanced adsorption/activation of reaction species, and reduced energy barrier for C & horbar;C coupling. Moreover, when explored in a membrane-electrode assembly electrolyzer, the Cu/Sr0.9TiO3-delta catalyst shows excellent activity, selectivity (43.9%), and stability for C2H4 at industrial current densities, being the most effective perovskite-based catalyst for CO2-to-C2H4 conversion.