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The lack of effective charge transfer driving force and channel limits the electron directional migration in nanoclusters (NC)-based heterostructures, resulting in poor photocatalytic performance. Herein, a Z-scheme NC-based heterojunction (Pt1Ag28-BTT/CoP, BTT = 1,3,5-benzenetrithiol) with strong internal electric field is constructed via interfacial Co–S bond, which exhibits an absolutely superiority in photocatalytic performance with 24.89 mmol·h−1·g−1 H2 production rate, 25.77% apparent quantum yield at 420 nm, and ~ 100% activity retention in stability, compared with Pt1Ag28-BDT/CoP (BDT = 1,3-benzenedithiol), Ag29-BDT/CoP, and CoP. The enhanced catalytic performance is contributed by the dual modulation strategy of inner core and outer shell of NC, wherein, the center Pt single atom doping regulates the band structure of NC to match well with CoP, builds internal electric field, and then drives photogenerated electrons steering; the accurate surface S modification promotes the formation of Co–S atomic-precise interface channel for further high-efficient Z-scheme charge directional migration. This work opens a new avenue for designing NC-based heterojunction with matchable band structure and valid interfacial charge transfer.
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