Conjugated microporous
polymers (CMPs) have gained much recent
attention as a kind of metal-free organic photocatalyst for photocatalytic
hydrogen generation. However, the development of a visible-light-driven
CMP photocatalyst with high photocatalytic activity is still a big
challenge. Here, we report dibenzothiophene dioxide containing CMP
photocatalysts and demonstrate the influence of the cross-linker length
on the photocatalytic performance for hydrogen production. The most
active photocatalyst of DBTD-CMP1 with a short cross-linker of benzene
exhibits a high hydrogen evolution rate (HER) of 2460 μmol h–1 g–1 under visible light without
Pt cocatalyst. Remarkably, the Pt-loaded DBTD-CMP1 shows an attractive
HER of 9200 μmol h–1 g–1 under UV–vis light illumination. This result demonstrates
that these dibenzothiophene dioxide containing CMPs are competitive
with the most reported porous organic polymer photocatalysts.
Recently, great progress has been achieved in the design and preparation of conjugated organic polymer photocatalysts for hydrogen generation. However, it is still challenging to develop an organic polymer photocatalyst with high photoconversion efficiency. Rational structure design of organic polymer photocatalysts holds the key point to realize high photocatalytic performance. Herein, a series of donor–π–acceptor (D–π–A) conjugated organic copolymer photocatalysts is developed using statistical copolymerization by tuning the feed molar ratio of pyrene (donor) to dibenzothiophene‐S,S‐dioxide (acceptor) units. It reveals that the photocatalytic activity of the resulting copolymers is significantly dependent on the molar ratio of donor to acceptor, which efficiently changes the polymer structure and component. When the monomer feed ratio is 25:75, the random copolymer PyBS‐3 of 10 mg with Pt cocatalyst shows a high hydrogen evolution rate of 1.05 mmol h−1 under UV/Vis light irradiation using ascorbic acid as the hole‐scavenger, and an external quantum efficiency of 29.3% at 420 nm, which represents the state‐of‐the‐art of organic polymer photocatalysts. This work demonstrates that statistical copolymerization is an efficient strategy to optimize the polymer structure for improving the photocatalytic activity of conjugated organic polymer catalysts.
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