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用于在铜单原子和铜簇的级联位点上将一氧化碳电还原为乙醇的压力增强型碳-碳偶联反应

Pressure-Boosted C-C Coupling for CO Electroreduction to Ethanol over the Cascade Sites of Cu Single-Atom and Cu Cluster.

作者信息

Wu Haoyang, Xu Wenhai, Tian Benqiang, Zou Jiaoling, Abdalla Kovan K, Li Mengxuan, Zhou Linlin, Li Boyuan, Yu Jiage, Wang Yuan, Li Jiazhan, Sun Xiaoming

机构信息

State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.

出版信息

Small. 2025 Jul;21(29):e2504102. doi: 10.1002/smll.202504102. Epub 2025 May 23.

DOI:10.1002/smll.202504102
PMID:40405754
Abstract

Tandem catalysis of the CO electroreduction reaction (CORR) offers a promising way to obtain multicarbon products (C) with high Faradaic efficiency (FE). However, the synchronously changed CO supply and consumption with potentials and the mismatch between the two potential windows of the different components in tandem catalysts impede further understanding and development of tandem catalysis. Herein, a novel strategy of pressure regulating to separately promote the CO supply and consumption is reported on the cascade sites of Cu single-atom and Cu cluster, where a near-linear relationship between CO pressure, CO supply, and ethanol FE is well established. Benefiting from the above strategy, the ethanol FE of 41.2% is achieved under 26 bar CO, which increases by ≈3 times that under ambient pressure. This work provides a new method of CO supply regulation and gives more mechanism insights into the tandem catalysis of CO electroreduction toward multicarbon products.

摘要

串联催化CO电还原反应(CORR)为获得具有高法拉第效率(FE)的多碳产物(C)提供了一条很有前景的途径。然而,CO的供应和消耗随电位同步变化,以及串联催化剂中不同组分的两个电位窗口之间的不匹配,阻碍了对串联催化的进一步理解和发展。在此,报道了一种在Cu单原子和Cu簇的级联位点上分别促进CO供应和消耗的压力调节新策略,其中CO压力、CO供应和乙醇FE之间建立了良好的近似线性关系。受益于上述策略,在26 bar CO下实现了41.2%的乙醇FE,比常压下提高了约3倍。这项工作提供了一种CO供应调节的新方法,并为CO电还原为多碳产物的串联催化提供了更多的机理见解。

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