Hydrogen Spillover-Bridged C–N Bond Cleavage of Pt-WO ₃ /REUSY for Accelerating HDN Activity

This study elucidates the enhanced hydrodenitrogenation (HDN) performance of PtW 10 /REUSY catalysts, driven by a synergistic hydrogen spillover mechanism. Experimental evidence from DRIFTS, visual colorimetry, and EPR confirms that activated hydrogen species (*H) migrate from Pt to WO 3, generating surface hydroxyls and unsaturated W 5+ sites. While moderate temperatures maximize oxygen vacancy formation, excessive spillover at ∼600 °C leads to site passivation. Density functional theory (DFT) calculations reveal that these W 5+ sites drastically lower C–N bond cleavage barriers─83.9 to 16.7 kcal/mol for decahydroquinoline─via dual-site adsorption. The optimized PtW 10 /REUSY catalyst achieves exceptional performance, with 99% quinoline conversion and an 80% denitrogenation rate at an ultralow temperature of 280 °C, representing an 80 °C reduction compared to conventional NiMo/Al 2 O 3 catalysts, which typically require temperatures above 360 °C to attain similar conversions. This work establishes a structure–activity relationship, highlighting the balance between spillover-induced activation and high-temperature saturation for optimizing HDN catalysts.