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Covalent Organic Frameworks Enabling Site Isolation of Viologen‐Derived Electron‐Transfer Mediators for Stable Photocatalytic Hydrogen Evolution
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2021-01-22 , DOI: 10.1002/anie.202016618 Zhen Mi 1 , Ting Zhou 1 , Weijun Weng 1 , Junjuda Unruangsri 2 , Ke Hu 3 , Wuli Yang 1 , Changchun Wang 1 , Kai A. I. Zhang 4 , Jia Guo 5
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2021-01-22 , DOI: 10.1002/anie.202016618 Zhen Mi 1 , Ting Zhou 1 , Weijun Weng 1 , Junjuda Unruangsri 2 , Ke Hu 3 , Wuli Yang 1 , Changchun Wang 1 , Kai A. I. Zhang 4 , Jia Guo 5
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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.
中文翻译：
共价有机框架可实现位置隔离的紫精衍生的电子转移介体，从而稳定地进行光催化氢的释放
电子转移是光催化水分解中的限速步骤。紫精及其衍生物能够充当电子转移介体（ETM），促进电子从光敏剂到活性位的快速转移。尽管如此，通过含阳离子基的紫罗兰碱衍生的ETM之间的耦合，电子转移能力经常会遭受稳定的偶极结构的形成，从而限制了电子转移过程。此处，环状敌草快是一种源自紫精的ETM，它通过季铵化后的反应被整合到基于2,2'-联吡啶的共价有机骨架（COF）中。嵌入式diquat-ETM的内容和分布受到严格控制，从而实现了有利的站点隔离安排。-1 g -1）和与单模块COF和COF / ETM混合物相比具有持久的性能。二维COF平台中应用的集成策略通过多组分合作促进了光化学过程中的连续电子转移。
更新日期：2021-01-22
中文翻译：
共价有机框架可实现位置隔离的紫精衍生的电子转移介体，从而稳定地进行光催化氢的释放
电子转移是光催化水分解中的限速步骤。紫精及其衍生物能够充当电子转移介体（ETM），促进电子从光敏剂到活性位的快速转移。尽管如此，通过含阳离子基的紫罗兰碱衍生的ETM之间的耦合，电子转移能力经常会遭受稳定的偶极结构的形成，从而限制了电子转移过程。此处，环状敌草快是一种源自紫精的ETM，它通过季铵化后的反应被整合到基于2,2'-联吡啶的共价有机骨架（COF）中。嵌入式diquat-ETM的内容和分布受到严格控制，从而实现了有利的站点隔离安排。-1 g -1）和与单模块COF和COF / ETM混合物相比具有持久的性能。二维COF平台中应用的集成策略通过多组分合作促进了光化学过程中的连续电子转移。
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