Customizing dumbbell-shaped heterostructured artificial photosystems steering versatile photoredox catalysis

定制哑铃形异质结构人工光系统以调控多功能光氧化还原催化

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Abstract

Benefiting from their excellent light-capturing ability, suitable energy band structure and abundant active sites, transition metal chalcogenides (TMCs) have been attracting widespread attention in heterogeneous photocatalysis. Nonetheless, TMCs still suffer from sluggish charge transfer kinetics, a rapid charge recombination rate and poor stability, rendering the construction of high-performance artificial photosystems challenging. Here, a ternary dumbbell-shaped CdS/MoS(2)/CuS heterostructure with spatially separated catalytically active sites has been elaborately designed. In such a heterostructured nanoarchitecture, MoS(2) clusters, selectively grown on both ends of the CdS nanowires (NWs), act as terminal electron collectors, while CuS nanolayers, coated on the sidewalls of CdS NWs through ion exchange, form a P-N heterojunction with the CdS NW framework, which accelerates the migration of holes from CdS to CuS, effectively suppressing the oxidation of sulfide ions and improving the stability of CdS NWs. The well-defined dumbbell-shaped CdS/MoS(2)/CuS ternary heterostructure provides a structural basis for spatially precise regulation of the charge migration pathway, where photogenerated electrons and holes directionally migrate to the MoS(2) and CuS catalytic sites, respectively, ultimately achieving efficient carrier separation and significantly enhancing photoactivity for both photocatalytic hydrogen generation and selective organic transformation under visible light. Moreover, we have also ascertained that such ion exchange and interface configuration engineering strategies are universal. Our work features a simple yet efficient strategy for smartly designing multi-component heterostructures to precisely modulate spatially vectorial charge separation at the nanoscale for solar-to-hydrogen conversion.

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