Differentiated adsorption of intermediates on high-entropy intermetallic metallene promotes selective electrocatalytic upgrading of PET plastics to glycolic acid
摘要
The electrocatalytic oxidation of ethylene glycol (EG) derived from polyethylene terephthalate (PET) waste to valuable glycolic acid (GA) represents an attractive route for waste resource upcycling. However, achieving high selectivity remains challenging due to the difficulty in steering the complex reaction pathway. In this study, PdPtCuInBi high-entropy intermetallic metallene (HEI-PdPtCuInBiene) is reported to precisely control EG oxidation reaction (EGOR) pathway for GA production by constructing multiple active sites at the atomic scale. In PET hydrolysate, it achieves a Faradaic efficiency of 99.87% and a production rate of 1.47 mmol h−1 cm−2, along with excellent stability. Mechanistic studies reveal that the high-entropy structure induces strong p-d orbital hybridization, which optimizes the electronic structure of active sites, thus weakening the adsorption of key carbonyl intermediates and suppressing C–C bond cleavage. The synergistic electronic effect among Pd, Pt, and Cu further enables differential adsorption of distinct intermediates on diverse active sites, enhancing the selective formation of GA. Techno-economic analysis exhibits high profitability (∼$784.9 t−1 PET) of this route, demonstrating the great potential of high-entropy intermetallic metallene in regulating electrocatalytic upcycling of PET waste and beyond.