期刊
ACS CATALYSIS
卷 9, 期 10, 页码 9438-9445出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b01951
关键词
covalent triazine framework; donor-acceptor; photoinduced electron transfer; charge recombination; photocatalytic hydrogen evolution
资金
- National Natural Science Foundation of China [21875078, 21604028]
- International S & T Cooperation Program of China [2016YFE0124400]
- Program for HUST Interdisciplinary Innovation Team [2016JCTD104]
- Analysis and Testing Center of Huazhong University of Science and Technology
Conjugated porous polymers (CPPs) have recently emerged as prospective materials for photocatalytic hydrogen evolution. In the design of CPP photocatalysts, one of the challenges is to find ways to inhibit backward charge recombination and promote forward charge transfer/separation. Conjugated donor-acceptor polymers are capable of favoring forward intramolecular charge separation; however, they often suffer from backward charge recombination simultaneously, which causes a decrease of the quantum efficiency for solar-energy conversion. Herein, a photoinduced electron-transfer system via constructing D-A(1)-A(2) conjugated polymers for photocatalytic hydrogen evolution is developed. Such a D-A(1)-A(2) system can not only boost charge separation but also suppress charge recombination owing to the cascade energy levels of the comprised units and large charge delocalization structures. Therefore, an apparent quantum yield up to 22.8% at 420 nm is achieved, and the highest hydrogen evolution rate can be up to 966 mu mol h(-1) (19.3 mmol g(-1) h(-1)) under visible light irradiation. These values are comparable to the state-of-the-art CPPs as well as part of inorganic photocatalysts. This work provides an alternative strategy and insight for the design of CPP photocatalytic systems for photocatalytic applications in high efficiency.
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