Molecular Engineering of Conjugated Polybenzothiadiazoles for Enhanced Hydrogen Production by Photosynthesis

作者：Can Yang, Beatriz Chiyin Ma, Linzhu Zhang, Sen Lin, Saman Ghasimi, Katharina Landfester, Kai A. I. Zhang, Xinchen Wang · 发表于：Angewandte Chemie International Edition · 年份：2016 · DOI：10.1002/anie.201603532 · 被引用次数：395 · 研究领域：Advanced Photocatalysis Techniques、Covalent Organic Framework Applications、Metal-Organic Frameworks: Synthesis and Applications

The search for metal-free organic photocatalysts for H2 production from water using visible light remains a key challenge. Reported herein is a molecular structural design of pure organic photocatalysts, derived from conjugated polybenzothiadiazoles, for photocatalytic H2 evolution using visible light. By alternating the substitution position of the electron-withdrawing benzothiadizole unit on the phenyl unit as a comonomer, various polymers with either one- or three-dimensional structures were synthesized and the effect of the molecular structure on their catalytic activity was investigated. Photocatalytic H2 evolution efficiencies up to 116 μmol h(-1) were observed by employing the linear polymer based on a phenyl-benzothiadiazole alternating main chain, with an apparent quantum yield (AQY) of 4.01 % at 420 nm using triethanolamine as the sacrificial agent.