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

ABSTRACT 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.