Site-Decoupled Electrocatalysis with Adaptive *OH Supply for Selective Polyethylene Terephthalate Upcycling.

Ethylene glycol (EG) serves as the primary hydrolysis product of polyethylene terephthalate (PET), making its electro-oxidation reaction (EGOR) a key pathway for high-value plastic waste utilization. However, conventional coupled strategy fails to meet the dual requirements of EG dehydrogenation and hydroxyl species (*OH) supply. This functional incompatibility hinders catalytic performance by limited intermediate conversion, inducing site poisoning and reducing GA selectivity. We design a site-decoupled strategy to address these problems, where Pt sites drive EG dehydrogenation while oxophilic Co oxyhydroxides facilitate hydroxylation via *OH supply. Crucial to this design is the Co-O-Pt bridging-oxygen structure, which establishes a rapid electronic coupling channel, optimizes intermediate adsorption, and accelerates charge transfer. The PtCo-Ni(OH)2@NF exhibits a mass activity of 9.87 A mg Pt-1 with 92.8% Faradaic efficiency and 97.3% selectivity toward GA, achieving a 6.8-fold enhancement in cumulative GA production over the coupled strategy. The system sustains operation for 300 h with negligible decay. Scalability tests using 100.0 g of real-world PET yielded 81.1 g PTA (93.8% yield) and 23.1 g GA (58.4% yield). Techno-economic analysis estimates a potential profit of ∼US$515.5 per ton of waste PET, demonstrating this strategy as a promising pathway for high-value upcycling of diverse polyester and polyol feedstocks.