A surface strategy boosting the ethylene selectivity for CO2 reduction and in situ mechanistic insights

Yinchao Yao, Tong Shi, Wenxing Chen, Jiehua Wu, Yunying Fan, Yichun Liu, Liang Cao () and Zhuo Chen ()
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Yinchao Yao: School of Materials Science and Engineering, Beijing Institute of Technology
Tong Shi: Zhejiang University
Wenxing Chen: School of Materials Science and Engineering, Beijing Institute of Technology
Jiehua Wu: SINOPEC (Beijing) Research Institute of Chemical Industry Co., Ltd
Yunying Fan: Kunming University of Science and Technology
Yichun Liu: Kunming University of Science and Technology
Liang Cao: Zhejiang University
Zhuo Chen: School of Materials Science and Engineering, Beijing Institute of Technology

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Electrochemical reduction of carbon dioxide into ethylene, as opposed to traditional industrial methods, represents a more environmentally friendly and promising technical approach. However, achieving high activity of ethylene remains a huge challenge due to the numerous possible reaction pathways. Here, we construct a hierarchical nanoelectrode composed of CuO treated with dodecanethiol to achieve elevated ethylene activity with a Faradaic efficiency reaching 79.5%. Through on in situ investigations, it is observed that dodecanethiol modification not only facilitates CO2 transfer and enhances *CO coverage on the catalyst surfaces, but also stabilizes Cu(100) facet. Density functional theory calculations of activation energy barriers of the asymmetrical C–C coupling between *CO and *CHO further support that the greatly increased selectivity of ethylene is attributed to the thiol-stabilized Cu(100). Our findings not only provide an effective strategy to design and construct Cu-based catalysts for highly selective CO2 to ethylene, but also offer deep insights into the mechanism of CO2 to ethylene.

Date: 2024
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DOI: 10.1038/s41467-024-45704-2

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