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Triggering of Low-Valence Molybdenum in Multiphasic MoS2 for Effective Reactive Oxygen Species (ROS) Output in Catalytic Fenton-like Reactions.

Utilization of photocatalytic reactions to trigger persistent large-scale reactions could be an alternative path for the practical solar energy conversion to relieve environmental pressure nowadays. We took view that photo-induction of transition states was critical for improving activity of catalytic reaction. Using density functional theory prediction, we herein found that the reaction Gibbs free energy of permonosulfate (PMS) activation can be rapidly reduced by the polyvalent molybdenum with low valence. We therefore constructed a multiphasic molybdenum dichalcogenide (MoS2) heterostructure-based photosystem that enabled generation of Mo transition states by visible light excitation. Based on the combined results of photo-electrochemical analysis, X-ray photoelectron spectroscopy (XPS), and in-situ electron paramagnetic resonance (EPR), we confirmed that optimized 2H/1T heterojunction permitted transport of excited interfacial electrons from the semiconductive 2H phase to metallic 1T phase, and synchronously partially reduced Mo(IV) to Mo(III) at interface. This intensified charge transfer between MoS2 and PMS-containing solution, thereby efficiently splitting PMS molecules into •OH and SO4•- radicals. In this system, the 2,4-dichlorophenoxyacetic acid (2,4-D), a type of refractory organic contaminate, can be rapidly degraded in 60 min at a rate constant of 6.20×10-2 min-1 using multiphasic MoS2 with a 1T to 2H ratio of 1:1.