文献类型：期刊文献

英文题名：Enhancing Electrocatalysis of CO2 to Ethanol via Intercalated Electron Boosters in an Atomically Dispersed Ca-N4-Doped Graphene Bilayer

作者：Xia, Yanyan[1];Bao, Yihui[1];Lu, Xinyi[1];Ye, Zhencheng[1];Mei, Yuhan[2,3];Chen, Houyang[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：2024

卷号：64

期号：4

起止页码：2016

外文期刊名：INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH

收录：;WOS:【SCI-EXPANDED(收录号:WOS:001369543700001)】；

基金：This work is supported by the Postdoctoral Program of Natural Science Foundation of Chongqing (CSTB2023NSCQ-BHX0159), the Natural Science Foundation of Chongqing (CSTB2023NSCQ-MSX0045), the Startup Foundation of Chongqing Institute of Green and Intelligent Technology, Chinese Academy of Sciences. Computations were performed on Hefei Advanced Computing Center. The authors acknowledge Beijing PARATERA Tech CO., Ltd for providing HPC resources that have contributed to the research results reported within this paper. URL: https://paratera.com.

语种：英文

摘要：We report the development of atomically dispersed Ca-N4-doped graphene bilayers with single intercalated alkaline earth metal (AEM) atoms, denoted as CaN4-AEM-CaN4, designed to enhance the electrocatalytic conversion of CO2 to C1 and C2 products. These catalysts significantly improve the CO2 reduction reaction (CO2RR) activity and fine-tune the selectivity between C1 and C2 pathways. Based on our theoretical findings, we propose an electron transfer mechanism where AEM atoms serve as electron donors across both layers during nonadsorbed intermediate processes and as electron boosters that facilitate electron transfer from the nonadsorbed to the adsorbed layer during adsorption, thereby enhancing catalytic performance. AEMs also influence the reaction pathways, promoting the formation of more valuable C2 products by adjusting selectivity. Among the CaN4-AEM-CaN4 systems, CaN4-Sr-CaN4 stands out with a superior limiting potential (-0.93 V), demonstrating exceptional electrochemical catalytic activity for CO2-to-ethanol conversion. This study underscores the potential of CaN4-AEM-CaN4 catalysts for enhancing multicarbon CO2RR and provides key insights into the electron transfer mechanisms that drive their activity and selectivity.