小提琴手
电子转移
光化学
化学
共价键
光催化
光诱导电子转移
共价有机骨架
电子传输链
阳离子聚合
催化作用
化学工程
有机化学
生物化学
工程类
作者
Zhen Mi,Ting Zhou,Weijun Weng,Junjuda Unruangsri,Ke Hu,Wuli Yang,Changchun Wang,Kai A. I. Zhang,Jia Guo
标识
DOI:10.1002/anie.202016618
摘要
Abstract Electron transfer is the rate‐limiting step in photocatalytic water splitting. Viologen and its derivatives are able to act as electron‐transfer mediators (ETMs) to facilitate the rapid electron transfer from photosensitizers to active sites. Nevertheless, the electron‐transfer ability often suffers from the formation of a stable dipole structure through the coupling between cationic‐radical‐containing viologen‐derived ETMs, by which the electron‐transfer process becomes restricted. Herein, cyclic diquats, a kind of viologen‐derived ETM, are integrated into a 2,2′‐bipyridine‐based covalent organic framework (COF) through a post‐quaternization reaction. The content and distribution of embedded diquat‐ETMs are elaborately controlled, leading to the favorable site‐isolated arrangement. The resulting materials integrate the photosensitizing units and ETMs into one system, exhibiting the enhanced hydrogen evolution rate (34600 μmol h −1 g −1 ) and sustained performances when compared to a single‐module COF and a COF/ETM mixture. The integration strategy applied in a 2D COF platform promotes the consecutive electron transfer in photochemical processes through the multi‐component cooperation.
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