Polyethylene Terephthalate Hydrolysis Catalyzed by Deep Eutectic Solvents: COSMO-RS Screening and Experimental Validation

Chemical recycling is one of the most prominent techniques that enables monomer recovery for plastics like polyethylene terephthalate (PET), which ultimately reduces the dependency on virgin material inputs. In this study, 40 deep eutectic solvents (DESs) were pre-screened using COSMO-RS to identify the best solvent for chemical recycling of PET. Quantitative evaluation was performed based on activity coefficients (γ) to assess solute–solvent interactions. Qualitatively, the sigma profile and sigma potential were analyzed to understand the polarity and affinity of each DES component. This study experimentally validated the two top-performing DESs based on COSMO-RS output. The DES formed by combining thymol with phenol (Thy/Phe (1:2)) achieved 100% PET degradation and 94.5% terephthalic acid (TPA) recovery from post-consumer PET in just 25 min. The rapid dissolution of PET into molten state accelerated the hydrolysis reaction, leading to efficient monomer recovery. The second DES, tetrabutylammonium bromide/sulfolane (TBABr/Sulf (1:7)), attained 93.7% PET degradation and 94% TPA recovery. The PET-to-solvent ratio used in this study was 0.75, while the PET-to-DES ratio in the mixture was only 0.15, the lowest reported for DES-assisted hydrolysis to date. Characterization of the recycled TPA confirmed a purity level comparable to its virgin grade, as verified by FT−IR analysis. This study presents two important outcomes. First, the use of COSMO-RS for DES selection provides a strong rationale for solvent choice in targeted reactions and processes. Second, the use of appropriate DES in this study helps reduce key parameters associated with depolymerisation process, including reaction time, temperature, and catalyst consumption.