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, Zhuo Chen
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 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.