Electron‐Enriched Pt‐In Synergistic Sites for Highly Selective and Direct Photo‐Reforming of PET Plastic Wastes into Acetic Acid

Abstract Photocatalytic selective upcycling of polyethylene terephthalate (PET) waste into valuable C 2 products is an ideal strategy. However, over‐oxidation and nonselective activation of C─C/C─O bonds by active sites in the local microenvironment have limited prior studies to produce C 2 products. By designing Pt/ZnO‐ZIS catalysts that feature a dynamically coupled Pt‐In dual‐site synergistic interface, this study achieves in situ upcycling of PET wastes via tuning the electronic structure and chemical environment of the Pt‐In active sites and optimizing the adsorption configuration of plastic wastes. The dual active sites (Pt‐In), which are spatially adjacent yet functionally distinct, achieves an HOAc production rate of 882.46 µmol g −1 h −1 with nearly 100% selectivity. Detailed characterizations and DFT calculations reveal that the high selectivity is attributed to the Pt sites adsorbing and protecting the terminal hydroxyl group (‐OH) oxidation, and then activating the C─O bond to undergo proton substitution. The electron‐rich Pt sites further inhibit the over‐oxidation of C─C bond, ensuring high selectivity of HOAc. Simultaneously, the In sites facilitate oxidation of ‐OH to form carboxyl species during the reaction. This study provides an insightful understanding of dual sites with dynamic reconstruction toward highly selective photo‐reforming of plastic wastes at the atomic scale.