Recycling of Waste PET into Terephthalic Acid in Neutral Media Catalyzed by the Cracking Zeolite/Alumina Binder Acidic Catalyst

This study addresses the critical issue of environmental pollution from plastic waste by investigating an effective chemical recycling method for polyethylene terephthalate (PET) via neutral catalytic hydrolysis. We utilized a recoverable and regenerable composite catalyst based on cracking zeolite and γ-Al2O3, which possesses both Brønsted and Lewis acidic sites that facilitate the depolymerization of PET into its constituent monomers, terephthalic acid (TPA) and ethylene glycol (EG). This investigation reveals that the catalytic performance is strongly dependent on the total acid site concentration and the specific nature of these sites. A key finding is that a balanced acidic profile with a high proportion of Brønsted acid sites is crucial for enhancing PET hydrolysis attributed to a significant decrease in the activation energy of the reaction. The experiments were conducted in a stirred stainless-steel autoclave reactor, where key parameters such as temperature (210–230 °C), the PET-to-water ratio (1:2 to 1:5), and reaction time were systematically varied. Under optimal conditions of 210 °C and a 6 h reaction time, the process achieved near-complete PET depolymerization (99.5%) and a high TPA yield (90.24%). The catalyst demonstrated remarkable recyclability, maintained its activity over multiple cycles and was easily regenerated. Furthermore, the recovered TPA was of high quality, with a purity of 98.74% as confirmed by HPLC, and exhibited a melt crystallization temperature 14 °C lower than that of the commercial standard. These results not only demonstrate the efficiency and sustainability of neutral catalytic hydrolysis using zeolite/alumina composites but also provide valuable insights for designing advanced catalysts with tunable acidic properties. By demonstrating the importance of tuning acidic properties, specifically the balance between Brønsted and Lewis sites, this work lays a foundation for developing more effective catalysts that can advance circular economy goals for PET recycling.