期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 40, 页码 22062-22069出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202109968
关键词
conjugated microporous polymers; heavy-atom free; heterogeneous catalysis; intersystem-crossing; photocatalytic oxidation
资金
- National Natural Science Foundation of China [22071180]
- Natural Science Foundation of Tianjin City of China [18JCJQJC47700]
Decorating conjugated microporous polymers with polycyclic aromatic hydrocarbons has improved photosensitization and facilitated efficient photosynthesis by promoting intersystem crossing and electron-hole separation. The structure-property-activity relationship of these polymers demonstrates a new approach for developing heavy-atom-free heterogeneous photosensitizers with highly efficient sensitizing activity at a molecular level.
Photosensitization associated with light absorption and energy/electron-transfer represents the central processes for photosynthesis. However, it's still a challenge to develop a heavy-atom-free (HAF) strategy to improve the sensitizing ability of polymeric photosensitizers. Herein, we propose a new protocol to significantly improve the photosensitization by decorating mother conjugated microporous polymer (CMP-1) with polycyclic aromatic hydrocarbons (PAHs), resulting in a series of CMPs (CMP-2-4). Systematic study reveals that covalent modification with PAHs can transfer charge to Bodipy in CMP to further facilitate both intersystem crossing and electron-hole separation, which can dramatically boost energy-/electron-transfer reactions. Remarkably, CMP-2 as a representative CMP can efficiently drive the photosynthesis of methyl phenyl sulfoxide with 92 % yield, substantially higher than that of CMP-1 (32 %). Experiments and theory calculations demonstrate the structure-property-activity relationship of these CMPs, opening a new horizon for developing HAF heterogeneous photosensitizers with highly efficient sensitizing activity by rational structure regulation at a molecular level.
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