Copper atom-pair catalyst anchored on alloy nanowires for selective and efficient electrochemical reduction of CO2

• Published in: Nature chemistry Vol. 11; no. 3; pp. 222 - 228
• Main Authors: Jiao, Jiqing, Lin, Rui, Liu, Shoujie, Cheong, Weng-Chon, Zhang, Chao, Chen, Zheng, Pan, Yuan, Tang, Jianguo, Wu, Konglin, Hung, Sung-Fu, Chen, Hao Ming, Zheng, Lirong, Lu, Qi, Yang, Xuan, Xu, Bingjun, Xiao, Hai, Li, Jun, Wang, Dingsheng, Peng, Qing, Chen, Chen, Li, Yadong
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 01-03-2019; Nature Publishing Group
• Subjects: 639/638/298; 639/638/77/886; Analytical Chemistry; Biochemistry; Carbon cycle; Carbon dioxide; Catalysis; Catalysts; Chemical reduction; Chemistry; Chemistry and Materials Science; Chemistry/Food Science; Climate change; Copper; Density functional theory; Electrochemistry; Hydrogen evolution reactions; Inorganic Chemistry; Nanotechnology; Nanowires; Organic Chemistry; Physical Chemistry; Selectivity; Single atom catalysts
• ISSN: 1755-4330; 1755-4349
• DOI: 10.1038/s41557-018-0201-x

The electrochemical reduction of CO
2
could play an important role in addressing climate-change issues and global energy demands as part of a carbon-neutral energy cycle. Single-atom catalysts can display outstanding electrocatalytic performance; however, given their single-site nature they are usually only amenable to reactions that involve single molecules. For processes that involve multiple molecules, improved catalytic properties could be achieved through the development of atomically dispersed catalysts with higher complexities. Here we report a catalyst that features two adjacent copper atoms, which we call an ‘atom-pair catalyst’, that work together to carry out the critical bimolecular step in CO
2
reduction. The atom-pair catalyst features stable Cu
1
0
–Cu
1
x
+
pair structures, with Cu
1
x
+
adsorbing H
2
O and the neighbouring Cu
1
0
adsorbing CO
2
, which thereby promotes CO
2
activation. This results in a Faradaic efficiency for CO generation above 92%, with the competing hydrogen evolution reaction almost completely suppressed. Experimental characterization and density functional theory revealed that the adsorption configuration reduces the activation energy, which generates high selectivity, activity and stability under relatively low potentials.
Anchored single-atom catalysts have recently been shown to be very active for various processes, however, a catalyst that features two adjacent copper atoms—which we call an atom-pair catalyst—is now reported. The Cu
1
0
–Cu
1
x
+
pair structures work together to carry out the critical bimolecular step in CO
2
reduction.