Taguchi Robust Design of Phase Transfer Catalytic Hydrolysis of Polyethylene Terephthalate (PET) Waste in Mild Conditions: Application for the Preparation of Metal–Organic Frameworks

Abstract

With the rapid increase in polyethylene terephthalate (PET) usage in recent years, recycling has become indispensable in mitigating environmental damage and safeguarding natural resources. In this context, this study presents a methodology for valorizing PET waste through phase transfer catalytic hydrolysis conducted at a low temperature (80 °C) and atmospheric pressure, with the goal of recovering the terephthalic acid (TPA) monomer. The recovered TPA monomer was subsequently utilized as a precursor for the synthesis of metal–organic frameworks (MOFs). Tributylhexadecyl phosphonium bromide (3Bu6DPB) was selected as the phase transfer catalyst due to its efficiency and sustainability. The process parameters, including the concentration of NaOH, the wt.% of catalyst to PET, and the concentration of PET in the solution, were varied to optimize the hydrolysis reaction. The Taguchi design methodology with an L9 (3^3) orthogonal array was employed to analyze the influence of these factors on the depolymerization time. The analysis of variance (ANOVA) results revealed that the concentration of NaOH was the most significant factor, contributing to 93.3% of the process efficiency, followed by the wt.% of the catalyst to PET (6.5%). The findings also demonstrated that the concentration of NaOH had the greatest impact (Δ = 4.27, rank = 1), while the concentration of PET had the smallest effect (Δ = 0.16, rank = 3). The optimal conditions for PET depolymerization were achieved in 75 min with 20 g/100 mL of NaOH, 12 wt.% of catalyst to PET, and 5 g/100 mL of PET. The recovered TPA monomer was further employed as an organic ligand to synthesize Fe(III)-TPA MOFs under mild conditions (80 °C for 24 h). The X-ray diffraction (XRD) analysis revealed the simultaneous formation of MOF-235(Fe) and MIL-101(Fe), two multifunctional materials with diverse properties and applications. This study highlights an efficient approach for producing low-cost MOFs while promoting urban waste recycling, contributing to an integrated strategy for PET recycling and resource valorization.