MIL‐125‐PDI/ZnIn2S4 Inorganic–Organic S‐Scheme Heterojunction With Hierarchical Hollow Nanodisc Structure for Efficient Hydrogen Evolution from Antibiotic Wastewater Remediation

Efficient photocatalytic production of H2 from wastewater is expected to address environmental pollution and energy crises effectively. However, the rapid recombination of photoinduced carriers results in low photoconversion efficiency. At present, inorganic–organic S‐scheme heterojunction have become a prominent and promising technology. In this study, an organic ligand modified MIL‐125‐PDI/ZnIn2S4 (ZIS) inorganic–organic S‐scheme heterojunction catalyst is designed. ZIS nanosheets are grown on the disc‐shaped MIL‐125‐PDI surface to form a distinctive hollow nanodiscs with hierarchical structure, giving the material an abundance of surface active sites, an optimized electronic structure, and a spatially separated redox surface. Consequently, the optimal 100MIL‐125‐PDI250/ZIS exhibited high photocatalytic HER of 508.99 µmol g−1 h−1 in Tetracycline hydrochloride (TC‐HCl) solution. Meanwhile, the catalyst achieved complete TC‐HCl removal and mineralization rate of 66.62% in 4 h. Experimental and theoretical calculations corroborate that the staggered band alignment and work function difference between MIL‐125‐PDI and ZIS induce the formation of a built‐in electric field, thus regulating the charge transfer routes and consequently enhancing charge separation efficiency. The possible photocatalytic mechanism is analyzed using liquid chromatography‐mass spectrometry (LC‐MS), and the toxicities of the degradation products are also evaluated. This work presents a green dual‐function strategy for H2 production and antibiotic wastewater recycling. Herein, a three‐layer dual‐functional MIL‐125‐PDI/ZIS organic–inorganic S‐scheme photocatalysts that achieves simultaneous H2 production and photocatalytic degradation of antibiotic contaminants in wastewater is designed. The material has an abundance of surface active sites, an optimized electronic structure, and a spatially separated redox surface. The catalyst exhibits excellent H2 production activity (508.99 µmol g−1 h−1) and degradation kinetic (2.16 h−1) in TC‐HCl solution (20 mg L−1).