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; Bin Liu

doi:10.1038/s41467-024-54636-w

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

Nat Commun. 2024 Nov 26;15(1):10247. doi: 10.1038/s41467-024-54636-w.

Authors

Shifu Wang^#^{1

2}, Fuhua Li^#^{3

4}, Jian Zhao², Yaqiong Zeng², Yifan Li⁵, Zih-Yi Lin⁶, Tsung-Ju Lee⁶, Shuhui Liu⁷, Xinyi Ren², Weijue Wang², Yusen Chen², Sung-Fu Hung⁶, Ying-Rui Lu⁸, Yi Cui⁵, Xiaofeng Yang², Xuning Li⁹, Yanqiang Huang^{10

11}, Bin Liu^{12

13}

Affiliations

¹ Department of Chemical Physics, University of Science and Technology of China, Hefei, 230026, P. R. China.
² State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, P. R. China.
³ Department of Materials Science and Engineering, City University of Hong Kong, Kowloon, Hong Kong SAR, 999077, China.
⁴ Department of Chemistry, Hong Kong Institute of Clean Energy (HKICE) & Center of Super-Diamond and Advanced Films (COSDAF), City University of Hong Kong, Kowloon, Hong Kong SAR, 999077, China.
⁵ Vacuum Interconnected Nanotech Workstation, Suzhou Institute of NanoTech and NanoBionics, Chinese Academy of Sciences, Suzhou, 215123, P. R. China.
⁶ Department of Applied Chemistry and Center for Emergent Functional Matter Science, National Yang Ming Chiao Tung University, Hsinchu, 300, Taiwan.
⁷ School of Computer and Communication Engineering, Dalian Jiaotong University, Dalian, 116028, P. R. China.
⁸ National Synchrotron Radiation Research Center, Hsinchu, 300, Taiwan.
⁹ State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, P. R. China. lixn@dicp.ac.cn.
¹⁰ Department of Chemical Physics, University of Science and Technology of China, Hefei, 230026, P. R. China. yqhuang@dicp.ac.cn.
¹¹ State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, P. R. China. yqhuang@dicp.ac.cn.
¹² Department of Materials Science and Engineering, City University of Hong Kong, Kowloon, Hong Kong SAR, 999077, China. bliu48@cityu.edu.hk.
¹³ Department of Chemistry, Hong Kong Institute of Clean Energy (HKICE) & Center of Super-Diamond and Advanced Films (COSDAF), City University of Hong Kong, Kowloon, Hong Kong SAR, 999077, China. bliu48@cityu.edu.hk.

^# Contributed equally.

PMID: 39592645
DOI: 10.1038/s41467-024-54636-w

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.

Abstract

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