Manipulating C-C coupling pathway in electrochemical CO2 reduction for selective ethylene and ethanol production over single-atom alloy catalyst

Shifu Wang, Fuhua Li, Jian Zhao, Yaqiong Zeng, Yifan Li, Zih-Yi Lin, Tsung-Ju Lee, Shuhui Liu, Xinyi Ren, Weijue Wang, Yusen Chen, Sung-Fu Hung, Ying-Rui Lu, Yi Cui, Xiaofeng Yang, Xuning Li (), Yanqiang Huang () and Bin Liu ()
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Shifu Wang: University of Science and Technology of China
Fuhua Li: City University of Hong Kong
Jian Zhao: Chinese Academy of Sciences
Yaqiong Zeng: Chinese Academy of Sciences
Yifan Li: Chinese Academy of Sciences
Zih-Yi Lin: National Yang Ming Chiao Tung University
Tsung-Ju Lee: National Yang Ming Chiao Tung University
Shuhui Liu: Dalian Jiaotong University
Xinyi Ren: Chinese Academy of Sciences
Weijue Wang: Chinese Academy of Sciences
Yusen Chen: Chinese Academy of Sciences
Sung-Fu Hung: National Yang Ming Chiao Tung University
Ying-Rui Lu: National Synchrotron Radiation Research Center
Yi Cui: Chinese Academy of Sciences
Xiaofeng Yang: Chinese Academy of Sciences
Xuning Li: Chinese Academy of Sciences
Yanqiang Huang: University of Science and Technology of China
Bin Liu: City University of Hong Kong

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Manipulation C-C coupling pathway is of great importance for selective CO2 electroreduction but remain challenging. Herein, two model Cu-based catalysts, by modifying Cu nanowires with Ag nanoparticles (AgCu NW) and Ag single atoms (Ag1Cu NW), respectively, are rationally designed for exploring the C-C coupling mechanisms in electrochemical CO2 reduction reaction (CO2RR). Compared to AgCu NW, the Ag1Cu NW exhibits a more than 10-fold increase of C2 selectivity in CO2 reduction to ethanol, with ethanol-to-ethylene ratio increased from 0.41 over AgCu NW to 4.26 over Ag1Cu NW. Via a variety of operando/in-situ techniques and theoretical calculation, the enhanced ethanol selectivity over Ag1Cu NW is attributed to the promoted H2O dissociation over the atomically dispersed Ag sites, which effectively accelerated *CO hydrogenation to form *CHO intermediate and facilitated asymmetric *CO-*CHO coupling over paired Cu atoms adjacent to single Ag atoms. Results of this work provide deep insight into the C-C coupling pathways towards target C2+ product and shed light on the rational design of efficient CO2RR catalysts with paired active sites.

Date: 2024
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DOI: 10.1038/s41467-024-54636-w

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