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Interfacial Electronic Coupling Engineering in Pt/WOx-Al2O3 for Hydrogen-Free Polyolefin Upcycling
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DOI：10.1039/D6TA02654K.png)
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Abstract
En 中文
Chemical upcycling of polyolefins under mild conditions is crucial for a circular polymer economy; yet achieving selective depolymerization without external hydrogen remains challenging. Herein; we report an interface-engineered bifunctional catalyst; Pt/W2.1–Al2O3; constructed by precisely regulating tungsten surface density and impregnation pH to tailor metal–oxide electronic coupling. The optimized catalyst enables complete polypropylene conversation at 250 oC with 59.4% selectivity toward C5–C22 (excluding C6) hydrocarbons under H2-free conditions.Operando spectroscopy reveals that interfacial dioxo (O=)2WO2 species electronically coupled with Ptδ+ clusters form cooperative active ensembles. This engineered interface promotes tandem β-scission and olefin metathesis. Meanwhile; the observed hydrogen spillover between Pt and WOx provides further evidence for Pt–WOx interfacial electronic interactions; while enhancing the reducibility of adjacent WOx species. This study establishes a surface hydroxyl-directed WOx anchoring strategy for regulating the WOx/γ-Al2O3 interface; thereby elucidating the structure–performance relationship between interfacial evolution and catalytic performance. The catalyst maintains structural integrity over ten cycles and efficiently upgrades diverse post-consumer plastics. This work highlights surface hydroxyl-directed WOx anchoring as an effective interfacial engineering strategy for designing efficient; durable; and hydrogen-independent catalysts for polyolefin upcycling.
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