文献类型：期刊文献

英文题名：CO2 electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment

作者：Ma, Zesong[1];Yang, Zhilong[1];Lai, Wenchuan[1];Wang, Qiyou[2];Qiao, Yan[1];Tao, Haolan[3,4];Lian, Cheng[3,4];Liu, Min[2];Ma, Chao[1];Pan, Anlian[1];Huang, Hongwen[1,5]

机构：[1]Hunan Univ, Coll Mat Sci & Engn, Changsha 410082, Hunan, Peoples R China;[2]Cent South Univ, Sch Phys & Elect, State Key Lab Powder Met, Changsha 410083, Hunan, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem & Mol Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai Engn Res Ctr Hierarch Nanomat, Shanghai 200237, Peoples R China;[5]Hunan Univ, Shenzhen Res Inst, Shenzhen, Guangdong, Peoples R China

年份：2022

卷号：13

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000969991400029)】；

基金：This work was supported by the National Key Research and Development Program of China (No. 2021YFA1502000 to H.H.), NSFC (No. U2032149 and 22102052 to H.H. and W.L.), the Science and Technology Innovation Program of Hunan Province (No. 2021RC3065 and 2021RC2053 to H.H. and W.L.), Hunan Provincial Natural Science Foundation of China (No. 2020JJ2001 to H.H.), Shenzhen Science and Technology Program (No. JCYJ20210324120800002 to H.H.), and the Hefei National Laboratory for Physical Sciences at the Microscale (No. KF2020108 to H.H.).

语种：英文

摘要：Electrochemical CO2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate CO2 electroreduction in strongly acidic electrolyte (pH <= 1) on electrochemically reduced porous Cu nanosheets by combining the confinement effect and cation effect to synergistically modulate the local microenvironment. A Faradaic efficiency of 83.7 +/- 1.4% and partial current density of 0.56 +/- 0.02 A cm(-2), single-pass carbon efficiency of 54.4%, and stable electrolysis of 30h in a flow cell are demonstrated for multicarbon products in a strongly acidic aqueous electrolyte consisting of sulfuric acid and KCl with pH <= 1. Mechanistically, the accumulated species (e.g., K+ and OH-) on the Helmholtz plane account for the selectivity and activity toward multicarbon products by kinetically reducing the proton coverage and thermodynamically favoring the CO2 conversion. We find that the K+ cations facilitate C-C coupling through local interaction between K+ and the key intermediate *OCCO.