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Electron delocalization in a fullerene-dumbbell triad: synergistically optimizing carrier dynamics for boosting photocatalytic hydrogen evolution
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DOI：10.1093/nsr/nwag479.png)
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Abstract
En 中文
Organic photocatalysts typically suffer from compromised carrier dynamics due to inherently low electron mobility and high exciton binding energy, limiting efficient photoconversion. Herein, we synergistically optimize carrier dynamics by modulating electron delocalization using a fullerene-based dumbbell-triad, B2, consisting of a dithienopyrrolobenzothiadiazole donor and two C60 acceptors. Steady-state and transient photoelectrochemical measurements confirm that, compared to the mono-fullerene-based B1 and the dodecyl-modified dumbbell-counterpart B3, B2 nanoparticles exhibit pronounced electron delocalization. This effect significantly reduces the exciton binding energy, enhances the electron mobility, prolongs the carrier lifetime and extends its intermolecular diffusion length, thereby synergistically optimizing charge-carrier generation, transport, and utilization. Consequently, B2 exhibits a markedly improved photocatalytic hydrogen evolution rate (136 mmol g−1 h−1), surpassing B1 by 17.4 times, positioning it competitively among high-performing single-component photocatalysts. This work provides a novel strategy for optimizing photogenerated carrier dynamics, and elucidates the critical role of electron delocalization in boosting photoconversion.
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