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Engineering a Copper Single-Atom Electron Bridge to Achieve Efficient Photocatalytic CO2 Conversion
Authors:Dr. Gang Wang  Yan Wu  Dr. Zhujie Li  Prof. Zaizhu Lou  Qingqing Chen  Yifan Li  Prof. Dingsheng Wang  Prof. Junjie Mao
Affiliation:1. Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002 P. R. China

These authors contributed equally to this work;2. Advanced Technology Research Institute, Beijing Institute of Technology, Jinan, 250300 P. R. China

These authors contributed equally to this work;3. Guangdong Provincial Key Laboratory of Nanophotonic Manipulation, Institute of Nanophotonics, Jinan University, Guangzhou, 511443 P. R. China;4. Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002 P. R. China;5. Department of Chemistry, Tsinghua University, Beijing, 100084 P. R. China

Abstract:Developing highly efficient and stable photocatalysts for the CO2 reduction reaction (CO2RR) remains a great challenge. We designed a Z-Scheme photocatalyst with N−Cu1−S single-atom electron bridge (denoted as Cu-SAEB), which was used to mediate the CO2RR. The production of CO and O2 over Cu-SAEB is as high as 236.0 and 120.1 μmol g−1 h−1 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−Cu1−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 CO2RR of Cu-SAEB. This work represents a promising platform for the development of highly efficient and stable photocatalysts that have potential in CO2 conversion applications.
Keywords:CO2RR  Electron Bridge  MIL-125-NH2  Single-Atom  Z-Scheme
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