文献类型：期刊文献

英文题名：Interlayer-confined-enabled dual-site synergy strategy: A bilayer FeN4 catalyst for enhanced CO2 reduction and C-C coupling

作者：Lu, Xinyi[1];Xia, Yanyan[1];Bao, Yihui[1];Ye, Zhencheng[1];Chen, Houyang[2,3];Huang, Haicai[2,3]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200237, Peoples R China;[2]Chinese Acad Sci, Chongqing Inst Green & Intelligent Technol, Chongqing 400714, Peoples R China;[3]Univ Chinese Acad Sci, Chongqing Sch, Chongqing 400714, Peoples R China

年份：2025

卷号：314

外文期刊名：CHEMICAL ENGINEERING SCIENCE

收录：;EI(收录号：20251918380291);WOS:【SCI-EXPANDED(收录号:WOS:001509845200001)】；

基金：This work is supported by the Postdoctoral Program of Natural Sci-ence Foundation of Chongqing (CSTB2023NSCQ-BHX0231) , Natural Science Foundation of Chongqing (CSTB2023NSCQ-MSX0045) , the

语种：英文

外文关键词：Interlayer confinement; Carbon-carbon coupling; Density functional theory; Single-site adsorption; Dual-site adsorption

摘要：We propose a dual-active-site catalytic system with an interlayer confinement effect, inducing a vertical synergistic interaction to enhance CO2 reduction reaction (CO2RR) activity and selectivity. Using density functional theory (DFT) calculations, we systematically explore how interlayer distance influences CO2 adsorption and key reaction intermediates. Our results reveal that confinement enhances electronic interactions, but excessive confinement induces steric hindrance, reducing catalytic activity. We identify two distinct carbon-carbon (C-C) coupling mechanisms: a single-site adsorption pathway involving *CO desorption followed by *CO + *CO coupling and a dual-site adsorption pathway enabled by *CHO rotation and subsequent *CO + *CHO coupling. Strong confinement enhances dual-site coupling. The optimal interlayer distance for ethanol production is 6.5 & Aring; (limiting potential: 0.7 V), while 7.5 & Aring; favors CH4 selectivity. This study establishes a theoretical framework for confined dual-site catalysis, providing design principles of interlayer-confined-enabled vertically aligned dualsite synergy approach for next-generation CO2 electrocatalysts.