期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 50, 页码 60072-60083出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c20579
关键词
photoredox catalysis; conjugated microporous polymers; donor structural design; carrier transfer; functionalization of thiophenols
资金
- National Science Foundation of China [51778226]
- Provincial Project of Research Study and Innovative Experiment for College Students [S202111342024]
- Hunan Natural Science Foundation for Distinguished Young Scholars [2021JJ10001]
- Hunan Science and Technology Talent Promotion Project [2020TJ-Q12]
- Hunan Provincial Natural Science Foundation [2019JJ50100, 2020JJ6013, 2021JJ50111, 2019JJ40057]
- Scientific Research Fund of Hunan Provincial Education Department [19A113]
The study presents a simple structural expansion strategy to facilitate charge transfer in conjugated microporous polymers, enhancing the efficiency of photogenerated carrier transfer and enabling high photocatalytic efficiency. This approach opens up new prospects for further optimization and rational design of photoactive polymers for efficient charge-transfer-mediated reactions.
Developing photocatalysts to steer conversion of solar energy toward high-value-added fine chemicals represents a potentially viable approach to address the energy crisis and environmental issues. However, enablement of this conversion is usually impeded by the sluggish kinetic process for proton-coupled electron transfer and rapid recombination of photogenerated excitons. Herein, we report a simple and general structural expansion strategy to facilitate charge transfer in conjugated microporous polymers (CMPs) via engineering the donor surrounding the trifluoromethylphenyl core. The resulting CMPs combine high surface area, strong light-harvesting capabilities, and tunable optical properties endowed by extended pi-conjugation; the optimized compound CbzCMP-5 generated from 9,9',9 ''-(2-(trifluoromethyobenzene-1,3,S-triyl)tris(9H-carbazole) remarkably enhanced the photogenerated carrier transfer efficiency, enabling the functionalization of thiophenols toward thiocarbamates and 3-sulfenylindoles with high photocatalytic efficiency. Most importantly, the in-depth insights into the carrier-transfer processes open up new prospects on further optimization and rational design of photoactive polymers for efficient charge-transfer-mediated reactions.
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