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 

机构地区：[1]State Key Laboratory of Catalysis,Collaborative Innovation Center of Chemistry for Energy Materials,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China [2]University of Chinese Academy of Sciences,Beijing 100049,China [3]Vacuum Interconnected Nanotech Workstation,Suzhou Institute of Nano-Tech and Nano-Bionics,Chinese Academy of Sciences,Suzhou 215123,Jiangsu,China

出　　处：《Journal of Energy Chemistry》2023年第10期102-107,I0005,共7页能源化学（英文版）

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)。

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.

关 键 词：CO electroreduction High pressure electrochemistry Cu catalyst C–C coupling Multicarbon products 

分 类 号：O643.32[理学—物理化学]