光化学
离域电子
共轭体系
光催化
电子转移
带隙
接受者
烷烃
共价键
材料科学
化学
聚合物
物理
有机化学
催化作用
光电子学
凝聚态物理
作者
Wenjuan Zhang,Lizheng Chen,Ruping Niu,Zhuoyuan Ma,Kaikai Ba,Tengfeng Xie,Xuefeng Chu,Shujie Wu,Dayang Wang,Gang Liu
标识
DOI:10.1002/advs.202308322
摘要
Abstract Constructing π‐conjugated polymer structures through covalent bonds dominates the design of organic framework photocatalysts, which significantly depends on the selection of multiple donor‐acceptor building blocks to narrow the optical gap and increase the lifetimes of charge carriers. In this work, self‐bipolarized organic frameworks of single aromatic units are demonstrated as novel broad‐spectrum‐responsive photocatalysts for H 2 O 2 production. The preparation of such photocatalysts is only to fix the aromatic units (such as 1,3,5‐triphenylbenzene) with alkane linkers in 3D space. Self‐bipolarized aromatic units can drive the H 2 O 2 production from H 2 O and O 2 under natural sunlight, wide pH ranges (3.0‐10.0) and natural water sources. Moreover, it can be extended to catalyze the oxidative coupling of amines. Experimental and theoretical investigation demonstrate that such a strategy obeys the mechanism of through‐space π‐conjugation, where the closely face‐to‐face overlapped aromatic rings permit the electron and energy transfer through the large‐area delocalization of the electron cloud under visible light irradiation. This work introduces a novel design concept for the development of organic photocatalysts, which will break the restriction of conventional through‐band π‐conjugation structure and will open a new way in the synthesis of organic photocatalysts.
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