Tensile-Strained Cu Penetration Electrode Boosts Asymmetric C-C Coupling for Ampere-Level CO2-to-C2+ Reduction in Acid

被引:12
作者
Li, Shoujie [1 ,3 ]
Wu, Gangfeng [1 ,2 ,3 ]
Mao, Jianing [2 ,4 ,5 ]
Chen, Aohui [1 ,3 ]
Liu, Xiaohu [1 ,3 ]
Zeng, Jianrong [5 ]
Wei, Yiheng [1 ,2 ,3 ]
Wang, Jiangjiang [1 ,2 ,3 ]
Zhu, Huanyi [1 ,2 ,3 ]
Xia, Jiayu [1 ,2 ,3 ]
Wang, Xiaotong [1 ,2 ,3 ]
Li, Guihua [1 ,3 ]
Song, Yanfang [1 ,2 ,3 ]
Dong, Xiao [1 ,2 ,3 ]
Wei, Wei [1 ,2 ,3 ]
Chen, Wei [1 ,2 ,3 ]
机构
[1] Chinese Acad Sci, Low Carbon Convers Sci & Engn Ctr, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Chinese Acad Sci, Shanghai Adv Res Inst, State Key Lab Low Carbon Catalysis & Carbon Dioxid, Shanghai 201210, Peoples R China
[4] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201204, Peoples R China
[5] Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
Acidic CO2 Electroreduction; Ampere-Level; Cu Penetration Electrode; Asymmetric C-C Coupling; Tensile-Strain; CO2; ELECTROREDUCTION; ELECTROCHEMICAL REDUCTION; CO2-TO-ETHANOL CONVERSION; MULTICARBON PRODUCTS; COPPER ELECTRODES; EVOLUTION; SELECTIVITY; EFFICIENT;
D O I
10.1002/anie.202407612
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The synthesis of multicarbon (C2+) products remains a substantial challenge in sustainable CO2 electroreduction owing to the need for sufficient current density and faradaic efficiency alongside carbon efficiency. Herein, we demonstrate ampere-level high-efficiency CO2 electroreduction to C2+ products in both neutral and strongly acidic (pH=1) electrolytes using a hierarchical Cu hollow-fiber penetration electrode (HPE). High concentration of K+ could concurrently suppress hydrogen evolution reaction and facilitate C-C coupling, thereby promoting C2+ production in strong acid. By optimizing the K+ and H+ concentration and CO2 flow rate, a faradaic efficiency of 84.5 % and a partial current density as high as 3.1 A cm(-2) for C2+ products, alongside a single-pass carbon efficiency of 81.5 % and stable electrolysis for 240 h were demonstrated in a strong acidic solution of H2SO4 and KCl (pH=1). Experimental measurements and density functional theory simulations suggested that tensile-strained Cu HPE enhances the asymmetric C-C coupling to steer the selectivity and activity of C2+ products.
引用
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页数:11
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