Synergistic promotion strategy of “dual-site” and “dual-path” to enhance the C–C coupling between CO_(2) and HCHO driven by photoelectrocatalysis  

作　　者：Hongqiang Yang Jianfeng Zheng Guoyu Wang Yifei Gao Yatao Yang Jia Li Xiaojin Han Yan Cui Zhanggen Huang 

机构地区：[1]National Key Laboratory of High Efficiency and Low Carbon Utilization of Coal,Institute of Coal Chemistry,Chinese Academy of Science,Taiyuan 030001,Shanxi,China [2]University of Chinese Academy of Science,Beijing 100049,China [3]Shenyang University of Chemical Technology,Shenyang 110142,Liaoning,China

出　　处：《Journal of Energy Chemistry》2025年第1期39-49,共11页能源化学(英文版)

基　　金：Natural Science Foundation of Shanxi Province,China (Grant No. 20210302123001);DNL Cooperation Fund,CAS (DNL202004),ICC CAS (Grant No. SCJCWRW-2023-21);Key Research and Development Program of Shanxi Province (202202090301020)。

摘　　要：Photoelectrocatalytic coupling CO_(2)and volatile organic compounds (VOCs) is a promising green strategy for the synergistic conversion of the two carbon-containing resources to C2products.The catalytic efficiency is always at the mercy of chemical inertness of CO_(2)and the competitive hydrogen evolution of H2O.Herein,a modified g-C_(3)N_(4)/ZnAl-LDH Z-scheme heterojunction catalyst with dual reaction site was rationally designed and precisely constructed.The Faraday efficiency of ethanol reached 68.67%with a corresponding formation rate of 227.3μmol g^(-1)h^(-1).As revealed by in-situ characterizations and density functional theory calculations,CO_(2)and HCHO were absorbed at Zn site and N site,respectively.Then,*CO generated from CO_(2)and HCHO was converted to*CH_(3)O and*CHO on the dual-active-site heterojunction.The detailed reaction mechanism experiments indicated that C–C coupling only occurred between*CO and*CH_(3)O in electrocatalysis process.Apart from the“*CO+*CH_(3)O”path,another“*CO+*CHO”coupling path was also detected in photoelectrocatalytic process.The selectivity of ethanol was significantly enhanced due to the synthesis of dual-site catalyst and the dual-path coupling path between CO_(2)and HCHO simultaneously driven by light and electricity.

关 键 词：g-C_(3)N_(4)/ZnAl-LDH heterojunction Z-scheme C-C coupling ETHANOL 

分 类 号：O643.36[理学—物理化学] X701[理学—化学]