Boosting C–C coupling to multicarbon products via high-pressure CO electroreduction

作     者：Wenqiang Yang Huan Liu Yutai Qi Yifan Li Yi Cui Liang Yu Xiaoju Cui Dehui Deng Wenqiang Yang;Huan Liu;Yutai Qi;Yifan Li;Yi Cui;Liang Yu;Xiaoju Cui;Dehui Deng

作者机构：State Key Laboratory of CatalysisCollaborative Innovation Center of Chemistry for Energy MaterialsDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of SciencesBeijing 100049China Vacuum Interconnected Nanotech WorkstationSuzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123JiangsuChina 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2023年第85卷第10期

页      面：102-107,I0005页

核心收录：

学科分类：081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 

基　　金：financial support from the National Key R&D Program of China (Nos. 2022YFA1504500, 2022YFA1503100) the National Natural Science Foundation of China (Nos. 21988101, 21890753, 22225204, 92145301, 22002160 and 22272174) the Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDB36030200) the CAS Project for Young Scientists in Basic Research (No. YSBR-028) the Fundamental Research Funds for the Central Universities (No. 20720220008) the Dalian National Lab for Clean Energy (DNL Cooperation Fund 202001) the Innovation Research Fund Project of DICP (No. DICP I202016) 

主　　题：CO electroreduction High pressure electrochemistry Cu catalyst C–C coupling Multicarbon products 

摘      要：Electrochemical CO reduction reaction(CORR) provides a promising approach for producing valuable multicarbon products(C_(2+)), while the low solubility of CO in aqueous solution and high energy barrier of C–C coupling as well as the competing hydrogen evolution reaction(HER) largely limit the efficiency for C_(2+)production in CORR. Here we report an overturn on the Faradaic efficiency of CORR from being HER-dominant to C_(2+)formation-dominant over a wide potential window, accompanied by a significant activity enhancement over a Moss-like Cu catalyst via pressuring CO. With the CO pressure rising from 1 to 40 atm, the C_(2+)Faradaic efficiency and partial current density remarkably increase from 22.8%and 18.9 mA cm^(-2)to 89.7% and 116.7 mA cm^(-2), respectively. Experimental and theoretical investigations reveal that high pressure-induced high CO coverage on metallic Cu surface weakens the Cu–C bond via reducing electron transfer from Cu to adsorbed CO and restrains hydrogen adsorption, which significantly facilitates the C–C coupling while suppressing HER on the predominant Cu(111) surface, thereby boosting the CO electroreduction to C_(2+)activity.