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The higher the polarity or the hydrogen bond donor ability of the solvent, the more easily COFs crystallize, and the higher the COF crystallization, the higher the photocatalytic H2 evolution.

A sulfide oxidation tuning approach in BDTT is reported for constructing a series of dual acceptor1-2 (A1–A2)-type copolymers. PBDTTS-1SO achieved an outstanding HER, demonstrating that the immense potential of the A1-A2-type polymer photocatalysts.

Photocatalytic water splitting is attracting considerable interest because it enables abundant solar energy to be converted into hydrogen for use as a zero-emission fuel or chemical feedstock. Herein, we present a universal approach for inserting hydrophilic non-conjugated building blocks into the main-chain of conjugated polymers to produce a series of discontinuously conjugated polymer (DCP) photocatalysts. Water can effectively be brought into the interior of DCPs through these hydrophilic non-conjugated building blocks, resulting in effective water/polymer interfaces inside the bulk DCPs in both thin-film and solution. P-10HEG with 10 mol% ethylene glycol-based hydrophilic building blocks achieved a record high apparent quantum yield of 17.82% under 460 nm monochromatic light irradiation in solution and an excellent hydrogen evolution rate of 16.8 mmol m− 2 h− 1 in thin-film. Molecular dynamics simulation shows a trend similar to that in experiments, which confirms that main-chain engineering increases the possibility of a water-DCP interaction. Unlike the previous strategy of maintaining a long conjugation length, our approach results in DCP photocatalysts with an interrupted conjugation length that remains efficient photocatalysis.