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Interfacial π···π-Hole Interactions Regulate Exciton Evolution for Long-Lived Charge-Separated States and Efficient Photocatalytic Hydrogen Production
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DOI：10.1021/acssuschemeng.6c03618.png)
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Abstract
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Regulating the exciton evolution behavior of linear conjugated polymers and constructing efficient exciton cascade evolution pathways to convert their dominant nonradiative recombination into long-lived charge-separated (CS) states remains a significant challenge. We propose a viable strategy centered on engineering interfacial π···π-hole interactions to modulate the exciton evolution processes and achieve long-lived CS states. Specifically, by compositing the poly(3,4-dimethoxythiophene-alt-4,7-dithienyl-2,1,3-benzothiadiazole) (PDB) with graphitic carbon nitride (CN), we fabricated 2D/2D PDB/CN heterojunctions with interfacial π···π-hole interactions. It is proven that the interfacial π···π-hole interactions not only regulate the exciton evolution pathways but also construct efficient charge transport channels, achieving long-lived CS states and excellent photocatalytic hydrogen production performance. Femtosecond and nanosecond transient absorption (fs-TA/ns-TA) spectroscopy analysis demonstrates that these interactions can accelerate the evolution of localized excitons (LE) to charge-transfer excitons (CT), suppress nonradiative recombination, and promote the conversion of CT states to long-lived CS states. This work reveals the crucial role of interfacial π···π-hole interactions in achieving long-lived CS states and provides important theoretical and experimental support for advancing the practical application of polymer photocatalysts.
Keywords:
linear conjugated polymers
exciton evolution
interfacial π···π-hole interactions
long-lived charge-separated states
2D/2D polymer heterojunctions
photocatalytic hydrogen production
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