Persistent radical cation sp2 carbon-covalent organic framework for photocatalytic oxidative organic transformations

被引：68
作者：
Cheng, Yuan-Zhe [1 ,3 ]
Ji, Wenyan [1 ]
Wu, Xianxin [2 ,3 ]
Ding, Xuesong [1 ]
Liu, Xin-Feng [2 ,3 ]
Han, Bao-Hang [1 ,3 ]
机构：
[1] Natl Ctr Nanosci & Technol, CAS Ctr Excellence Nanosci, CAS Key Lab Nanosyst & Hierarch Fabricat, Beijing 100190, Peoples R China
[2] Natl Ctr Nanosci & Technol, CAS Ctr Excellence Nanosci, CAS Key Lab Standardizat & Measurement Nanotechno, Beijing 100190, Peoples R China
[3] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
来源：
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2022年 / 306卷
基金：
中国国家自然科学基金;
关键词：
Sp(2) carbon-covalent organic framework; Photoinduced radical material; Photocatalyst; Charge separation and recombination; Porous organic polymer; HYDROXYLATION; ACIDS;
D O I：
10.1016/j.apcatb.2022.121110
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
Persistent radical covalent organic frameworks (COFs) have exhibited great application potential in the fields of photocatalysis, magnetism, and biology. However, there is still a lack of a simple, green, and effective way to produce persistent radical COFs. Here, we synthesized two sp2 carbon-covalent organic frameworks (sp(2)C-COFs) with persistent triphenylamine radical cation (TPA(+& BULL;)), which can be generated by simple light irradiation since the effective donor-acceptor heterojunction is formed in ordered skeleton. The number of persistent TPA(+& BULL;) will increase with the intensity of light irradiation and the photogenerated electrons generated simultaneously can be consumed by O-2 to form reactive oxygen species, which can be then used to carry out the oxidative organic transformations under visible light. In addition, femtosecond-transient absorption spectra prove that the difference in the structure of the two radical cation sp(2)C-COFs will significantly influence the charge recombination rate, so that the materials show different catalytic efficiency.
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页数：11
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