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

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.