Molecular Engineering of Conjugated Polybenzothiadiazoles for Enhanced Hydrogen Production by Photosynthesis

摘要

The search for metal-free organic photocatalysts for H-2 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 H-2 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 threedimensional structures were synthesized and the effect of the molecular structure on their catalytic activity was investigated. Photocatalytic H-2 evolution efficiencies up to 116 mu mol 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.