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构建铜单原子电子桥以实现高效光催化CO转化

Engineering a Copper Single-Atom Electron Bridge to Achieve Efficient Photocatalytic CO Conversion.

作者信息

Wang Gang, Wu Yan, Li Zhujie, Lou Zaizhu, Chen Qingqing, Li Yifan, Wang Dingsheng, Mao Junjie

机构信息

Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, P. R. China.

Advanced Technology Research Institute, Beijing Institute of Technology, Jinan, 250300, P. R. China.

出版信息

Angew Chem Int Ed Engl. 2023 Mar 20;62(13):e202218460. doi: 10.1002/anie.202218460. Epub 2023 Feb 20.

Abstract

Developing highly efficient and stable photocatalysts for the CO reduction reaction (CO RR) remains a great challenge. We designed a Z-Scheme photocatalyst with N-Cu -S single-atom electron bridge (denoted as Cu-SAEB), which was used to mediate the CO RR. The production of CO and O over Cu-SAEB is as high as 236.0 and 120.1 μmol g  h in the absence of sacrificial agents, respectively, outperforming most previously reported photocatalysts. Notably, the as-designed Cu-SAEB is highly stable throughout 30 reaction cycles, totaling 300 h, owing to the strengthened contact interface of Cu-SAEB, and mediated by the N-Cu -S atomic structure. Experimental and theoretical calculations indicated that the SAEB greatly promoted the Z-scheme interfacial charge-transport process, thus leading to great enhancement of the photocatalytic CO RR of Cu-SAEB. This work represents a promising platform for the development of highly efficient and stable photocatalysts that have potential in CO conversion applications.

摘要

开发用于一氧化碳还原反应(CO RR)的高效稳定光催化剂仍然是一项巨大挑战。我们设计了一种具有N-Cu -S单原子电子桥的Z型光催化剂(表示为Cu-SAEB),用于介导CO RR。在没有牺牲剂的情况下,Cu-SAEB上CO和O的生成速率分别高达236.0和120.1 μmol g  h,优于大多数先前报道的光催化剂。值得注意的是,由于Cu-SAEB的接触界面得到加强,并由N-Cu -S原子结构介导,所设计的Cu-SAEB在30个反应循环(总计300 h)中具有高度稳定性。实验和理论计算表明,SAEB极大地促进了Z型界面电荷传输过程,从而导致Cu-SAEB的光催化CO RR显著增强。这项工作为开发在CO转化应用中具有潜力的高效稳定光催化剂提供了一个有前景的平台。

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