文献类型：期刊文献

英文题名：Regulating Excitonic Effects in Covalent Organic Frameworks to Promote Free Charge Carrier Generation

作者：Liu, Fulai[1,5];He, Yanyan[2];Liu, Xiaopeng;Wang, Zhuan[4];Liu, Hong-Lai[6,7];Zhu, Xiang[2];Hou, Chun-Chao[1,5];Weng, Yuxiang[4];Zhang, Qianfan[3];Chen, Yong[1,5,8]

机构：[1]Chinese Acad Sci, Tech Inst Phys & Chem, Key Lab Photochem Convers & Optoelect Mat, Beijing 100190, Peoples R China;[2]Chinese Acad Sci, Lanzhou Inst Chem Phys, State Key Lab Oxo Synth & Select Oxidat, Suzhou Res Inst, Suzhou 215123, Peoples R China;[3]Beihang Univ, Sch Mat Sci & Engn, Beijing 100191, Peoples R China;[4]Chinese Acad Sci, Key Lab Soft Matter Phys Inst Phys, Beijing Natl Lab Condensed Matter Phys, CAS, Beijing, Peoples R China;[5]Chinese Acad Sci, Key Lab Soft Matter Phys Inst Phys, CAS, Beijing 100190, Peoples R China;[6]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[7]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[8]Univ Chinese Acad Sci, Beijing 100049, Peoples R China

年份：2022

卷号：12

期号：15

起止页码：9494

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20223512632954);WOS:【SCI-EXPANDED(收录号:WOS:000838228800001)】；

基金：The authors thank the financial support from the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB17000000) and the Natural Science Foundation of China (22102086, 21773275, and 21971250) . Y.C. thanks the financial support from the CAS-Croucher Funding Scheme for Joint Laboratories. X.Z. was supported by financial support from the National Program for Young Talents of China, the Foundation research project of Jiangsu Province (Y91266JZQ1) , and the National Natural Science Foundation of China (E00966GZQ2 and E00966GMS1) .

语种：英文

外文关键词：photocatalysis. covalent organic frameworks; excitonic effects; donor-acceptor interactions; charge carriers; photocatalysis

摘要：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.