Electrocatalytic Valorization of PET Hydrolysates Into High‐Value Chemicals Coupled With Renewable Energy Generation

ABSTRACT Electrocatalysis offers a sustainable pathway for upcycling polyethylene terephthalate (PET) waste. However, existing approaches often rely on high precious‐metal loadings and suffer rapid deactivation, limiting scalability. Herein, we report a full‐molecule valorization strategy for PET hydrolysates. PET‐derived benzene‐1,4‐dicarboxylate (BDC) is upcycled into a bifunctional Pt/Ni‐BDC catalyst, thereby reducing noble‐metal loading while achieving a remarkable current density of 378.8 mA cm ⁻² for ethylene glycol (EG) oxidation at 1.0 V vs. RHE with 90% glycolic acid (GA) selectivity. Mechanistic studies reveal that the Ni‐BDC framework enhances EG adsorption, thereby boosting performance. Additionally, the catalyst demonstrates excellent hydrogen evolution reaction activity, requiring only 39.6 mV to reach 50 mA cm ⁻² , outperforming commercial Pt/C. As a proof‐of‐concept, the catalyst was employed as the bifunctional electrode in a membrane‐free electrolyzer, enabling continuous electrochemical hydrogen production coupled with EG oxidation at ampere‐level current. The resulting GA was subsequently polymerized into biodegradable polyglycolic acid (PGA). Moreover, we developed an open‐loop flow battery integrating Pt/Ni‐BDC, which enables simultaneous electricity generation and GA production, delivering a discharge capacity of 3.53 Ah L ⁻¹ and an energy efficiency of 81%. By achieving full‐molecule valorization of PET hydrolysates, this work delivers a multifunctional platform for closed‐loop plastic valorization and green‐energy generation.