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

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.