Competitive Anchoring of Mo Atoms Induces Pt Atoms Agglomeration and Enhanced Electronic Effects: Elevated Activity and Selectivity for Carbon Disulfide Hydrogenation

Abstract High‐electron‐density Pt ⁰ nanoparticles (NPs) with excellent hydrogen activation and spillover capacity offer unique advantages in volatile organic sulfur selective hydrogenation reactions. Taking advantage of the more preferential and effective anchoring of Mo atoms at the γ‐Al ₂ O ₃ terminal hydroxyl (OH) groups and its electron modification role, competitive anchoring is induced by a simple co‐impregnation synthesis method to promote the agglomeration of low‐loading Pt atoms into high concentrations of electron‐rich and enlarged Pt NPs, which resulted in a substantial increase in the active centers for hydrogen dissociation. The Mo doping amount with the best Pt aggregation efficiency is 3 wt.%, and the hydrogen spillover efficiency of 1Pt3Mocom/Al catalyst is significantly higher than that of 1Pt/Al catalyst, which efficiently convert carbon disulfide (CS ₂ ) (95%–100%) while maintaining a methanethiol (CH ₃ SH) selectivity of 85% at 250 °C or a methane (CH ₄ ) selectivity of 92% at 310 °C in the 24 h long‐term test. In situ DRIFTS revealed that the improved catalyst performance is due to the elevated capacity to generate the intermediates HCSS ^* , CH ₂ S ^* , and CH ₃ S ^* . The 1Pt3Mocom/Al catalyst synthesized by competitive anchoring strategy greatly reduces the Pt consumption and is instructive for the exploitation of low‐cost Pt NPs active centers.