Статья

Dual donor-acceptor covalent organic frameworks for hydrogen peroxide photosynthesis

Chencheng QinCollege of Environmental Science and Engineering and Key Laboratory of Environmental Biology and Pollution Control (Ministry of Education), Hunan University, Changsha, 410082, ChinaXiaodong WuCollege of Materials Science and Engineering, Nanjing Tech University, Nanjing, 210009, ChinaLin TangCollege of Environmental Science and Engineering and Key Laboratory of Environmental Biology and Pollution Control (Ministry of Education), Hunan University, Changsha, 410082, ChinaXiaohong ChenSchool of Frontier Crossover Studies, Hunan University of Technology and Business, Changsha, 410205, ChinaMiao LiCollege of Environmental Science and Engineering and Key Laboratory of Environmental Biology and Pollution Control (Ministry of Education), Hunan University, Changsha, 410082, ChinaYi MouCollege of Environmental Science and Engineering and Key Laboratory of Environmental Biology and Pollution Control (Ministry of Education), Hunan University, Changsha, 410082, ChinaBo SuState Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fujian, 350002, ChinaSibo WangState Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fujian, 350002, ChinaChengyang FengCatalysis Centre, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Saudi ArabiaJiawei LiuSchool of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 21 Nanyang Link, 637371, Singapore, SingaporeXingzhong YuanCollege of Environmental Science and Engineering and Key Laboratory of Environmental Biology and Pollution Control (Ministry of Education), Hunan University, Changsha, 410082, China. [email protected]Yanli ZhaoSchool of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 21 Nanyang Link, 637371, Singapore, Singapore. [email protected]Hou WangCollege of Environmental Science and Engineering and Key Laboratory of Environmental Biology and Pollution Control (Ministry of Education), Hunan University, Changsha, 410082, China. [email protected]

2023en

ABI

Аннотация

Abstract Constructing photocatalytically active and stable covalent organic frameworks containing both oxidative and reductive reaction centers remain a challenge. In this study, benzotrithiophene-based covalent organic frameworks with spatially separated redox centers are rationally designed for the photocatalytic production of hydrogen peroxide from water and oxygen without sacrificial agents. The triazine-containing framework demonstrates high selectivity for H 2 O 2 photogeneration, with a yield rate of 2111 μM h −1 (21.11 μmol h −1 and 1407 μmol g −1 h −1 ) and a solar-to-chemical conversion efficiency of 0.296%. Codirectional charge transfer and large energetic differences between linkages and linkers are verified in the double donor-acceptor structures of periodic frameworks. The active sites are mainly concentrated on the electron-acceptor fragments near the imine bond, which regulate the electron distribution of adjacent carbon atoms to optimally reduce the Gibbs free energy of O 2 * and OOH* intermediates during the formation of H 2 O 2 .

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Идентификаторы

DOI: 10.1038/s41467-023-40991-7

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Цитирований: 2Использованных источников: 0

Показатели — AkademScholar