Ligand Functionalization Regulation in Metal–Organic Frameworks for Waste PET Valorization Coupled With Energy‐Saving Hydrogen Production

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Electrochemical conversion of PET‐derived ethylene glycol (EG) into value‐added chemicals provides a sustainable strategy for plastic‐waste valorization, but its practical implementation is limited by inefficient electrodes. Here, we report amino‐functionalized two‐dimensional Co‐BDC nanosheet arrays (Co‐BDC‐NH 2 ) as a highly efficient and robust anode for the electrochemical EG oxidation reaction (EGOR). The Co‐BDC‐NH 2 delivers an industrially relevant current density of 1000 mA cm −2 at only 1.36 V versus RHE, with a Faradaic efficiency of 95.6% toward formate. Mechanistic studies reveal that the electron‐donating amino ligands modulate the electronic structure of Co centers and the catalytic microenvironment, thereby promoting EG activation and selective C–C bond cleavage. When assembled into a two‐electrode EGOR||HER electrolyzer, the system lowers the cell voltage by 510 mV at 1000 mA cm −2 compared with conventional water electrolysis and operates continuously for 200 h with a low voltage degradation rate of 15 μV h −1 . The generated formate can be further converted into high‐value potassium diformate through mild acidification, highlighting the potential for value‐added chemical production from plastic‐derived feedstocks.