Rapid Surface Reconstruction of Amorphous‐Crystalline NiO for Industrial‐Scale Electrocatalytic PET Upcycling

Abstract The conversion of plastic waste into valuable chemicals through innovative and selective nano‐catalysts offers significant economic benefits and positive environmental impacts. However, our current understanding of catalyst design capable of achieving industrial‐grade current densities is limited. Herein, we develop a self‐supported amorphous‐crystalline NiO electrocatalyst for the electrocatalytic upcycling of polyethylene terephthalate (PET) into formate and hydrogen fuel. The catalyst achieves an industrial current density of over 1 A cm −2 at 1.5 V vs. RHE, with an 80 % Faradaic efficiency and a formate production rate of 7.16 mmol cm −2 h −1 . In situ Raman spectroscopy, X‐ray absorption spectroscopy, and density functional theory calculations reveal that the rapid transformation of amorphous‐crystalline NiO into γ‐NiOOH at the amorphous‐crystalline interface provides a thermodynamic advantage for formate desorption, leading to the high activity required for industrial applications, which is challenging to achieve for fully crystalline NiO. A techno‐economic analysis indicates that recycling waste PET using this catalytic process could generate a profit of $582 per ton. This work presents a cost‐effective and highly efficient approach to promoting the sustainable utilization of waste PET.