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Molecular Engineering Of Fully-Conjugated Sp2 Carbon-Linked Polymers For High-Efficiency Photocatalytic Hydrogen Evolution.

Jinlin Long, T. Huang, Xi Lin, Y. Liu, Jiwu Zhao, H. Lin, Ziting Xu, Shuncong Zhong, Xuxu Wang, X. Fu, C. Zhang
Published 2019 · Materials Science, Medicine

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The manifold organic precursors offer a versatile platform for precisely tailoring the electronic properties of semiconducting polymers. In this study, three fully-conjugated sp 2 carbon-linked polymers were designed and synthesized for photocatalytic hydrogen evolution under visible-light illumination, by copolymerizing different C3-symmetric aromatic aldehydes as knots with the 1,4-phenylene diacetonitrile (PDAN) linker through the -C=C- condensation reaction. A maximum hydrogen evolution rate (HER) of 30.2 mmol g -1 h -1 was achieved over the polymer CTTP based on 2,4,6-triphenyl-1,3,5-triazine units linked by cyano substituted phenylene, with an apparent quantum yield (AQY) of 7.20 % at 420 nm. Increasing the degree of conjugation and planarity not only extended the visible-light absorption, but also stabilized the fully-conjugated sp 2 carbon-linked donor-acceptor (D-A) polymer. Incorporating additional electron-withdrawing triazine units into the D-A polymer to form multiple electron donors and acceptors can greatly promote exciton separation and charge transfer, thus significantly enhance the photocatalytic activity.
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