期刊
ACS CATALYSIS
卷 12, 期 15, 页码 9494-9502出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c02173
关键词
photocatalysis. covalent organic frameworks; excitonic effects; donor-acceptor interactions; charge carriers; photocatalysis
资金
- Chinese Academy of Sciences [XDB17000000]
- Natural Science Foundation of China [22102086, 21773275, 21971250]
- CAS-Croucher Funding Scheme for Joint Laboratories
- National Program for Young Talents of China
- Foundation research project of Jiangsu Province [Y91266JZQ1]
- National Natural Science Foundation of China [E00966GZQ2, E00966GMS1]
This research presents a strategy of built-in control of donor-acceptor interactions to regulate excitonic effects in benzobisthiazole-bridged covalent organic frameworks, leading to accelerated exciton dissociation and enhanced photocatalytic activity for H2 evolution.
Strong excitonic effects, induced by the Coulombic interactions between photogenerated electrons and holes, seriously hinder the generation of free charge carriers in organic semiconductors for conducting photocatalysis. Herein, we report a built-in control of the donor-acceptor (D-A) interaction strategy to regulate excitonic effects within benzobisthiazole-bridged covalent organic frameworks (Tz-COFs). Theoretical calculation and ultrafast spectroscopy reveal that strengthening D-A interactions by this built-in control strategy in Tz-COFs can accelerate exciton dissociation, thus generating more long-lived photo-generated charge carriers for photoredox reactions. As a result, the optimized Tz-COF-3 exhibits high photocatalytic H2 evolution activity as high as 43.2 mmol g(-1) h(-1), with an apparent quantum yield of 6.9% at 420 nm. This work guides the development of COFs from excitonic aspects for photocatalysis.
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