PET Waste‐Derived Bimetallic MOFs Nanowire Arrays Enable Efficient Overall Water Splitting

Upcycling plastic waste into high‐value functional materials provides a compelling strategy to mitigate environmental pollution while enabling sustainable energy technologies, yet it remains a considerable challenge. Although polyethylene terephthalate (PET)‐derived metal‐organic frameworks (MOFs) have shown encouraging electrocatalytic performance, most are obtained as powders, and their direct growth on conductive substrates is still difficult. Herein, we report a facile synthesis of PET‐derived bimetallic NiM‐based MOF (M  Zn, Co, Cu) nanowire arrays as highly efficient oxygen‐evolving electrocatalysts. Theoretical calculations reveal that bimetallic MOFs exhibit an upshifted d ‐band center relative to monometallic counterparts, indicating enhanced interactions between active sites and reaction intermediates, which are critical for improved catalytic activity. Among them, NiCu‐MOF‐15 delivers bifunctional performance toward both the oxygen evolution reaction (OER) and urea oxidation reaction (UOR), achieving overpotentials of 375 and 201 mV to deliver 0.5 A cm −2 , respectively. Moreover, NiCu‐MOF‐15 enables efficient overall water electrolysis across a broad temperature range, requiring only 1.64 V to reach 0.5 A cm −2 at 80°C. Operando Raman spectroscopic analyses identify an in situ‐formed amorphous NiOOH layer as the active phase during OER and UOR. This work establishes an effective route for transforming PET waste into high‐performance MOF electrocatalysts and provides new insights into coupling plastic waste valorization with sustainable energy conversion.