Tuning structure and electronegativity of adjacent atoms of ZnIn2S4/Agx@GSH via Zn modification for enhanced photocatalytic hydrogen production Chemical Engineering Journal Volume 519, 1 September 2025, 165095
https://doi.org/10.1016/j.cej.2025.165095
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Designing efficient photocatalysts for photocatalysis hydrogen production is crucial for advancing green energy technologies. In this work, ZnIn2S4 photocatalyst with an asymmetric Zn-Zn-S unit ring structure and abundant in S vacancies was achieved by precisely tuning the molar mass of the Zn ion source using ethylene glycol as the reaction solvent. Z-type heterojunction was constructed via the electrostatic assembly by combining silver clusters (Agx@GSH) with ZnIn2S4 to enhance charge separation and photocatalytic activity. The structural transition from S-Zn-S to Zn-Zn-S led to local charge redistribution. Meanwhile, S vacancies acted as electron traps, promoting the charge state change of S in the SH sites and significantly accelerates the hydrogen evolution reaction (HER). The composite catalyst Zn-Vₛ-ZIS/Agx@GSH exhibited a hydrogen production rate of 18.4 mmol·g−1·h−1, under acidic conditions with lactic acid as the sacrificial agent, which is 3.7 times higher than pristine ZnIn2S4. Density functional theory (DFT) calculations revealed that the Zn-Zn-S distortion and heterojunction formation synergistically enhanced charge transfer and hydrogen adsorption kinetics. This work provides a novel approach for tailoring ZnIn2S4-based photocatalysts and provides new insights into the design of high-performance heterojunction systems for solar energy conversion.
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