Construction of S-scheme UiO-66-NH2/Zn0.4Cd0.6S hybrid architectures with strong interfacial interactions triggering efficient photocatalytic H2O2 production, nitrogen fixation, and water splitting

Abstract

Herein, UiO-66-NH₂ nanoparticles were solvothermally immobilized onto Zn_0.4Cd_0.6S nanorods in varying amounts. The resulting UiO-66-NH₂/Zn_0.4Cd_0.6S hybrid architectures demonstrated UiO-66-NH₂ content-dependent photocatalytic activity for visible-light-driven hydrogen peroxide (H₂O₂) production from pure water. Notably, the optimized UiO-66-NH₂/Zn_0.4Cd_0.6S-0.2 catalyst achieved the highest H₂O₂ yield under visible-light illumination, surpassing those of pure UiO-66-NH₂ and bare Zn_0.4Cd_0.6S by factors of 81.12 and 2.22, respectively. In addition, the UiO-66-NH₂/Zn_0.4Cd_0.6S-0.2 sample exhibited outstanding photocatalytic efficiency, achieving an NH₃ concentration of 25.02 ± 0.68 mg·L⁻¹ after 1 h of visible-light exposure and an H₂ evolution of 487.12 mmol g⁻¹ following 3 h of irradiation. The notable enhancement in the photocatalytic performance was attributed to efficient S-scheme charge transfer, as confirmed by transient absorption spectroscopy. The S-scheme charge migration mechanism in the UiO-66-NH₂/Zn_0.4Cd_0.6S system was further validated by electron paramagnetic resonance, density functional theory calculations, and in situ irradiated X-ray photoelectron spectroscopy. Overall, this study presents a promising strategy for designing highly efficient hybrid architectures for photocatalytic applications.