Electrochemical CO2 Reduction to C2+ Products with Ampere-Level Current on Carbon-Modified Copper Catalysts

被引:0
|
作者
Dong, Xue [1 ]
Sun, Xiaofu [2 ]
Jia, Shuaiqiang [1 ]
Han, Shitao [1 ]
Zhou, Dawei [1 ]
Yao, Ting [1 ]
Wang, Min [1 ]
Fang, Minghui [1 ]
Wu, Haihong [1 ]
Han, Buxing [1 ,2 ]
机构
[1] East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 200062, Peoples R China
[2] Chinese Acad Sci, CAS Res Educ Ctr Excellence Mol Sci, Beijing Natl Lab Mol Sci, Inst Chem,CAS Key Lab Colloid Interface & Chem The, Beijing 100190, Peoples R China
关键词
CO2; reduction; Electrocatalysis; Multi-carbon products; Green chemistry; Ampere-level current; ELECTROREDUCTION; DIOXIDE;
D O I
10.3866/PKU.WHXB202404012
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Copper-based electrocatalysts have great potential to produce high- value products in CO2 reduction reaction (CO2RR), offering a promising way to achieve negative carbon emissions. Additionally, achieving ampere-level currents is crucial for realizing the industrialization of multi-carbon (C2+) products. However, the C 2+ selectivity at industrial current densities remains unsatisfactory due to complex electron transport processes and inevitable side reactions. Herein, we developed a carbon-modification strategy aimed at optimizing the local environment and regulating the adsorption of intermediates at Cu active sites. Our findings demonstrated the effectiveness of Cu-Cx catalysts (where 'x' denoted the atomic percentage of C in the catalysts) in facilitating CO2RR for producing C 2+ products. Especially, over Cu-C6%, the current density could reach to 1.25 A center dot cm-2 at -0.72 V vs . RHE ( versus reversible hydrogen electrode) in a flow cell, and the Faradaic efficiency (FE) of C2H4 and C 2+ products could reach to 54.4% and 80.2%, respectively. In situ spectral analysis and density functional theory (DFT) calculations showed that the presence of C regulated the adsorption of * CO on Cu surface, reduced the energy barrier of C & horbar;C coupling, thus promoting the production of C 2+ products.
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页数:8
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