Alloying Strategy for the Electro‐Upcycling of Polyethylene Terephthalate (PET) to C 2 Products at Industrial‐Grade Current Density for over 700 h

Abstract As environmental pollution caused by polyethylene terephthalate (PET) waste continues to intensify, the electro‐upcycling of ethylene glycol (EG) derived from PET waste into value‐added products presents an efficient pathway to achieve “waste‐to‐treasure”. However, oxidation‐prone single‐metal sites and complex oxidation pathways of the EG oxidation reaction (EGOR) result in the deactivation of noble‐metal catalysts and poor selectivity toward C 2 products. Herein, an alloying strategy is developed to synthesize PtPd nanoparticles anchored on Ni(OH) 2 support (denoted as PtPd‐Ni(OH) 2 ). This approach exhibits an excellent EGOR activity (0.69 V RHE at ≈200 mA cm ‒2 ) with a high Faradaic efficiency of 90.38% for glycolic acid (GA) and steady electrolysis for over 700 h. In situ characterizations and density function theory (DFT) results reveal that the exceptional catalytic activity originates from the synergistic interaction of multicomponent systems, which optimizes the adsorption/desorption of oxidized intermediates and enhances the generation of * OH active species. Additionally, the construction of PtPd sites avoids the over‐oxidation of metallic sites and exhibits a wide potential range (0.3 V RHE –1.3 V RHE ). This work elucidates the underlying EGOR mechanism and enables the development of highly active, selective, and stable catalysts aiming at the complexity of the oxidation pathway, offering an efficient strategy for electrochemical upcycling of PET plastics.