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Engineering Plasmon-Semiconductor Coupling in Spatially Ordered Supraparticles for Boosted Photocatalytic Hydrogen Evolution
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PRE
AI
W
Z
姜
J
S
M
王
DOI：10.1002/anie.8359659.png)
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Abstract
En 中文
Organizing distinct nanocomponents into spatially ordered architectures offers a powerful strategy to regulate light-matter interactions and enhance photocatalytic efficiency, yet remains largely underexplored. Herein, we report the bottom-up construction of colloidal supraparticles (SPs) comprising photocatalytic CdS-based and plasmonic Au nanoparticles (NPs), forming spatially ordered hybrid superstructures with tunable Au NP size and compositional ratios. The optimized CdSe@CdS-Au SPs achieve a hydrogen evolution rate of 160 mmol h−1 g−1 under visible light, representing a significant enhancement over the mixture of the same components and outperforming previously reported similar NP-based systems. Ultrafast spectroscopic analyses combined with finite element simulations reveal that spatial confinement facilitates plasmon-mediated interactions between Au and CdSe@CdS NPs, leading to enhanced plasmonic local electric fields and efficient plasmon-induced resonance energy transfer from Au to the semiconductor domains. These photophysical advantages collectively account for the markedly improved photocatalytic activity. This study demonstrates nanoscale spatial engineering as a versatile strategy for tailoring hybrid architectures toward high-efficiency solar-to-chemical energy conversion.
Keywords:
photocatalytic HER performance
plasmonic-semiconductor NP assembly
resonance energy transfer
spatially ordered superstructure
synergic enhanced LSPR effect
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