Molecular Engineering of Conjugated Polybenzothiadiazoles for Enhanced Hydrogen Production by Photosynthesis.
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.
State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350002, P.R. China.
Can
C
Yang
Max Planck Institute for Polymer Research, Ackermannweg 10, 55128, Mainz, Germany.
Beatriz Chiyin
BC
Ma
State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350002, P.R. China.
Linzhu
L
Zhang
State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350002, P.R. China.
Sen
S
Lin
Max Planck Institute for Polymer Research, Ackermannweg 10, 55128, Mainz, Germany.
Saman
S
Ghasimi
Max Planck Institute for Polymer Research, Ackermannweg 10, 55128, Mainz, Germany.
Katharina
K
Landfester
Max Planck Institute for Polymer Research, Ackermannweg 10, 55128, Mainz, Germany. kai.zhang@mpip-mainz.mpg.de.
Kai A I
KA
Zhang
State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350002, P.R. China. xcwang@fzu.edu.cn.
Xinchen
X
Wang
D002384:Catalysis; D006859:Hydrogen / Q000737:chemistry*; D008027:Light; D010788:Photosynthesis; D011108:Polymers / Q000737:chemistry*; D013830:Thiadiazoles / Q000737:chemistry*
D011108:Polymers; D013830:Thiadiazoles; C015700:benzo-1,2,3-thiadiazole; D006859:Hydrogen
conjugation; hydrogen evolution; photocatalysis; polymers; semiconductors