AbstractHighly dispersed Pt‐bimetallic sub‐nanometer catalysts are crucial for efficient propane dehydrogenation (PDH), but synthesizing them with cost‐effective Pt precursors is challenging due to Pt's tendency to agglomerate, reducing catalytic activity. This study presents a Cs+‐mediated vacancy‐anchoring strategy to fabricate sub‐nanometer Pt‐bimetallic aggregates (CsPtM, M = Sn, V, Cr, Zn, Ga, Mn, Nb, Cu, and In) supported on Al₂O₃. Cs+ ions selectively occupy cationic vacancies on the Al₂O₃ surface, which serves to anchor Pt species, preventing their agglomeration and promoting the formation of sub‐nanoclusters through electrostatic interactions with [PtCl₆]2− precursor. Consequently, the CsPtM catalysts exhibit superior PDH performance compared to their PtM counterparts. Notably, CsPtSn demonstrates exceptional durability (450 h) and high propylene space–time yields (STY) after continuous operation. This enhanced performance is attributed to the strong metal‐support interaction induced by the vacancy‐anchoring strategy, which effectively suppresses metal sintering and preserves highly dispersed active sites.
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