Ampere-Level Current Density CO2 Reduction with High C2+ Selectivity on La(OH)3-Modified Cu Catalysts

被引:31
作者
Hu, Shuqi [1 ,2 ]
Chen, Yumo [1 ,2 ]
Zhang, Zhiyuan [1 ,2 ]
Li, Shaohai [1 ,2 ]
Liu, Heming [1 ,2 ]
Kang, Xin [1 ,2 ]
Liu, Jiarong [1 ,2 ]
Ge, Shiyu [1 ,2 ]
Wang, Jingwei [1 ,2 ]
Lv, Wei [1 ,2 ]
Zeng, Zhiyuan [3 ,4 ,5 ]
Zou, Xiaolong [1 ,2 ]
Yu, Qiangmin [1 ,2 ]
Liu, Bilu [1 ,2 ]
机构
[1] Tsinghua Univ, Tsinghua Berkeley Shenzhen Inst, Shenzhen Geim Graphene Ctr, Tsinghua Shenzhen Int Grad Sch, Shenzhen 518055, Peoples R China
[2] Tsinghua Univ, Inst Mat Res, Tsinghua Shenzhen Int Grad Sch, Shenzhen 518055, Peoples R China
[3] City Univ Hong Kong, Dept Mat Sci & Engn, Kowloon, 83 Tat Chee Ave, Hong Kong 999077, Peoples R China
[4] City Univ Hong Kong, State Key Lab Marine Pollut, P, R China, 83 Tat Chee Ave, Hong Kong 999077, Peoples R China
[5] City Univ Hong Kong, Shenzhen Res Inst, Shenzhen 518057, Peoples R China
基金
中国国家自然科学基金;
关键词
ampere-level current density; CO2; reduction; Cu; high C2+ selectivity; La(OH)(3); CARBON-DIOXIDE; ELECTROREDUCTION; CONVERSION; OXIDATION;
D O I
10.1002/smll.202308226
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The carbon dioxide reduction reaction (CO2RR) driven by electricity can transform CO2 into high-value multi-carbon (C2+) products. Copper (Cu)-based catalysts are efficient but suffer from low C2+ selectivity at high current densities. Here La(OH)(3) in Cu catalyst is introduced to modify its electronic structure towards efficient CO2RR to C2+ products at ampere-level current densities. The La(OH)(3)/Cu catalyst has a remarkable C2+ Faradaic efficiency (FEC2+) of 71.2% which is 2.2 times that of the pure Cu catalyst at a current density of 1,000 mA cm(-2) and keeps stable for 8 h. In situ spectroscopy and density functional theory calculations both show that La(OH)(3) modifies the electronic structure of Cu. This modification favors *CO adsorption, subsequent hydrogenation, *CO & horbar;*COH coupling, and consequently increases C2+ selectivity. This work provides a guidance on facilitating C2+ product formation, and suppressing hydrogen evolution by La(OH)(3) modification, enabling efficient CO2RR at ampere-level current densities.
引用
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页数:8
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