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

. 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.