Abstract
Photocatalytic aerobic oxidative desulfurization (PAODS) presents a promising and carbon-neutral avenue for desulfurizing petroleum products. However, existing photocatalysts encounter limitations in activating oxygen and show sluggish kinetics in sulfide-to-sulfone conversion, hampering widespread implementation. Herein, we present a FeMo6Ox nanocluster-modified CuS photocatalyst for PAODS reaction using air as an oxygen source. Through experimental characterization and density functional theory (DFT) calculations, we elucidate that the incorporation of FeMo6Ox nanoclusters can modulate the CuS electron density, which results in the generation of electron trap states and facilitates the separation of electron-hole pairs. We show that the variation of water content in air alters the generation efficiency of different reactive oxygen species (ROS), highlighting the potential to optimize moisture levels for achieving the highest catalytic efficiency. The optimized catalytic system exhibits a record specific activity of 10.42 mmol g−1 h−1, and more importantly, achieves deep desulfurization of authentic diesel, showcasing its appealing application prospects.
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