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

• Published in: Nature communications Vol. 15; no. 1; p. 1257
• Main Authors: Yao, Yinchao, Shi, Tong, Chen, Wenxing, Wu, Jiehua, Fan, Yunying, Liu, Yichun, Cao, Liang, Chen, Zhuo
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group 10.02.2024; Nature Publishing Group UK; Nature Portfolio
• Subjects: Carbon dioxide; Catalysts; Chemical reduction; Copper oxides; Density functional theory; Electrochemistry; Ethylene; Flat surfaces; Selectivity
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-024-45704-2

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 CO 2 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 CO 2 to ethylene, but also offer deep insights into the mechanism of CO 2 to ethylene.