Hu Shuqi, Chen Yumo, Zhang Zhiyuan, Li Shaohai, Liu Heming, Kang Xin, Liu Jiarong, Ge Shiyu, Wang Jingwei, Lv Wei, Zeng Zhiyuan, Zou Xiaolong, Yu Qiangmin, Liu Bilu
Shenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute & Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, P. R. China.
Department of Materials Science and Engineering, and State Key Laboratory of Marine Pollution, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong, 999077, P. R. China.
Small. 2024 Apr;20(14):e2308226. doi: 10.1002/smll.202308226. Epub 2023 Nov 16.
The carbon dioxide reduction reaction (CORR) driven by electricity can transform CO into high-value multi-carbon (C) products. Copper (Cu)-based catalysts are efficient but suffer from low C selectivity at high current densities. Here La(OH) in Cu catalyst is introduced to modify its electronic structure towards efficient CORR to C products at ampere-level current densities. The La(OH)/Cu catalyst has a remarkable C Faradaic efficiency (FE) of 71.2% which is 2.2 times that of the pure Cu catalyst at a current density of 1,000 mA cm and keeps stable for 8 h. In situ spectroscopy and density functional theory calculations both show that La(OH) modifies the electronic structure of Cu. This modification favors *CO adsorption, subsequent hydrogenation, *CO─*COH coupling, and consequently increases C selectivity. This work provides a guidance on facilitating C product formation, and suppressing hydrogen evolution by La(OH) modification, enabling efficient CORR at ampere-level current densities.
由电驱动的二氧化碳还原反应(CORR)可以将CO转化为高价值的多碳(C)产物。铜(Cu)基催化剂效率很高,但在高电流密度下C选择性较低。在此,在Cu催化剂中引入La(OH),以改变其电子结构,从而在安培级电流密度下实现高效的CORR生成C产物。La(OH)/Cu催化剂具有71.2%的显著C法拉第效率(FE),在电流密度为1000 mA cm时是纯Cu催化剂的2.2倍,并能稳定8小时。原位光谱和密度泛函理论计算均表明,La(OH)改变了Cu的电子结构。这种改变有利于*CO吸附、随后的氢化、*CO─*COH偶联,从而提高了C选择性。这项工作为促进C产物形成以及通过La(OH)改性抑制析氢提供了指导,从而在安培级电流密度下实现高效的CORR。