Efficient and sustainable recycling of polyethylene terephthalate (PET) is essential in mitigating its environmental impacts on climate, human health, and global ecosystems. Glycolysis, a closed-loop recycling method that converts PET into bis(2-hydroxyethyl) terephthalate (BHET), stands out as one of the most promising methods due to its mild operating conditions and environmentally friendly nature. However, the complete convert PET into BHET with a high stability are still challenging. In this study, magnetically recyclable CoFe2O4 nanocatalysts were synthesized by the solvothermal method and surface-modulated with Na3Cit·2H2O as a modifier. When utilizing an optimized CoFe2O4 catalyst, conversion of PET achieved 100 %, with a BHET yield of 91.7 % at 210 °C for 1 h. The excellent catalytic performance of CoFe2O4 is attributed to its smaller particle size, improved dispersion, higher surface Co/Fe ratio, and increased oxygen vacancies, all of which can be achieved through straightforward surface modulation. DFT calculations of M−O distance (M = Co or Fe), adsorption energy, and Bader charges confirm that a higher surface Co/Fe ratio enhanced PET glycolysis, consistent with experimental results. Additionally, a modified energy economy coefficient (εm) was proposed to characterize the catalytic efficiency. The εm value of CoFe2O4-60 % was 0.624, indicating promising applications in efficient PET glycolysis. This work presents a versatile approach for easily manipulating the surface properties of magnetic catalysts and identifies key factors for achieving high performance in PET-to-BHET conversion. It offers valuable guidelines for the future design of nanoparticle catalysts with magnetic properties for chemocatalytic reactions.
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