Bioinspired Design of F–Zn Sites in Layered Double Hydroxides for Photothermal Catalytic Upcycling of Polyethylene Terephthalate

Chemical upcycling of plastic wastes into high-value-added products presents a promising pathway toward achieving a circular economy and mitigating environmental issues, yet huge challenges remain. Drawing inspiration from hydrolases, this study proposes the construction of F-Zn sites in layered double hydroxides (LDHs) for the efficient photothermal catalytic upcycling of polyethylene terephthalate (PET) waste into bis(2-hydroxyethyl) terephthalate (BHET). Light irradiation induces dynamically varied Zn active sites, which mimic the metal centers of hydrolases and thereby facilitate the nucleophilic addition-elimination reaction at the carbonyl moieties of PET. Simultaneously, the high electronegativity of F intensifies its interaction with the hydroxyl groups of ethylene glycol. This mimics the hydrogen-bonding interactions mediated by the amino acid residues of hydrolases, promoting the nucleophilic attack on the PET. The synergistic effect of F-Zn configuration thereby effectively reduces the reaction energy barrier for PET glycolysis, enabling complete PET conversion under 160°C with a BHET yield of ∼80%. This study presents the integration of a bioinspired site-design strategy into a photothermal catalytic platform as a promising strategy for plastic waste upcycling.