Typical organic semiconductors show a high trap density of states (10 16 -10 18 cm À 3 ), providing a large number of centers for charge-carrier recombination, thus hindering the development of photocatalytic hydrogen evolution. Here, we design and synthesize a two-dimensional polycyclic photovoltaic material, named as TPP, to reduce the trap density to as low as 2.3 × 10 15 cm À 3 , which is 1-3 orders of magnitude lower than those of typical organic semiconductors. Moreover, TPP exhibits a broad and strong absorption, ordered molecular packing with a large crystalline coherence length and enhanced electron mobility. Then, the bulk heterojunction nanoparticles (BHJ-NPs) based on a blend of polymer donor (PM6) and TPP exhibit an average hydrogen evolution rate (HER) of 64.31 mmol h À 1 g À 1 under AM1.5G sunlight (100 mW cm À 2 ), and 72.75 mmol h À 1 g À 1 under 330-1100 nm illumination (198 mW cm À 2 ) higher than that of the control NPs based on typical PM6 : Y6 (62.67 mmol h À 1 g À 1 ).
The short exciton diffusion length (L
D) associated with most classical organic photocatalysts
(5–10
nm) imposes severe limits on photocatalytic hydrogen evolution efficiency.
Here, a photovoltaic molecule (F1) without electron-deficient units
at the central building block was designed and synthesized to improve
the photoluminescence quantum yield (PLQY). With the enhanced PLQY
of 9.3% and a large integral spectral overlap of 3.32 × 1016 nm4 M–1 cm–1, the average L
D of F1 film increases
to 20 nm, nearly twice the length of the control photovoltaic molecule
(Y6). Then, the single-component organic nanoparticles (SC-NPs) based
on F1 show an optimized average hydrogen evolution rate (HER) of 152.60
mmol h–1 g–1 under AM 1.5G sunlight
(100 mW cm–2) illumination for 10 h, which is among
the best results for photocatalytic hydrogen evolution.
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