Photosensitive Hyper-Cross-Linked Polymers Derived from Three-Dimensional Ringlike Arenes: Promising Catalysts for Singlet-Oxygen Generation,ACS Sustainable Chemistry & Engineering

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Photosensitive Hyper-Cross-Linked Polymers Derived from Three-Dimensional Ringlike Arenes: Promising Catalysts for Singlet-Oxygen Generation
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-10-23 , DOI: 10.1021/acssuschemeng.0c06025
Guipeng Ji ₁ , Zhenzhen Yang ₁ , Xiaoxiao Yu _{1,

2} , Yanfei Zhao _{1,

2} , Fengtao Zhang _{1,

2} , Zhimin Liu _{1,

2}

Affiliation

Solar energy-driven synthesis of chemicals is of great significance for green and sustainable development, and design of photocatalysts with high efficiency is an interesting topic. Herein, a series of hyper-cross-linked polymers (PS-HCPs) with excellent photosensitivity were synthesized via one-pot polymerization of non-photosensitive arenes with three-dimensional ringlike stereostructures (e.g., hexaphenylbenzene) under AlCl₃ catalysis in dichloromethane. They could efficiently convert O₂ into singlet oxygen under visible light irradiation and showed excellent activity for catalyzing aerobic photooxidation of benzylamines, sulfides, and benzyl alcohols to corresponding target products in high yields. Especially, PS-HCP-4 derived from hexaphenylbenzene even showed 2 times higher activity for benzylamine photooxidation than the best polymer-based photocatalyst to date. In addition, the resultant PS-HCP catalysts were stable and could be reused for 5 times without obvious activity loss.

中文翻译：

三维环状芳烃衍生的光敏超交联聚合物：单线态氧生成的有前途的催化剂

太阳能驱动的化学合成对绿色可持续发展具有重要意义，高效设计光催化剂是一个有趣的话题。本文中，通过在二氯甲烷中的AlCl ₃催化下，通过具有三维环状立体结构（例如，六苯基苯）的非光敏芳烃的一锅聚合，合成了一系列具有优异光敏性的超交联聚合物（PS-HCP）。他们可以有效地转换O ₂在可见光照射下转化为单线态氧，并显示出优异的催化活性，可高产率地催化苄胺，硫化物和苄醇氧化为相应的目标产物。特别是，衍生自六苯基苯的PS-HCP-4的苄胺光氧化活性甚至比迄今为止最好的聚合物基光催化剂高2倍。另外，所得的PS-HCP催化剂是稳定的并且可以重复使用5次而没有明显的活性损失。

更新日期：2020-11-02

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