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PETG (poly(ethylene glycol-co-cyclohexane-1,4-dimethanol terephthalate)) is an amorphous copolymer, biocompatible, recyclable, and versatile. Nowadays, it is being actively researched for biomedical applications. However, proposals of PETG as a platform for the loading of bioactive compounds from natural extract are scarce, as well as the effect of the supercritical impregnation on this polymer. In this work, the supercritical impregnation of PETG filaments with Olea europaea leaf extract was investigated, evaluating the effect of pressure (100–400 bar), temperature (35–55 °C), and depressurization rate (5–50 bar min−1) on the expansion degree, antioxidant activity, and mechanical properties of the resulting filaments. PETG expansion degree ranged from ~3 to 120%, with antioxidant loading ranging from 2.28 to 17.96 g per 100 g of polymer, corresponding to oxidation inhibition values of 7.65 and 66.55%, respectively. The temperature and the binary interaction between pressure and depressurization rate most affected these properties. The mechanical properties of PETG filaments depended greatly on process variables. Tensile strength values were similar or lower than the untreated filaments. Young's modulus and elongation at break values decreased below ~1000 MPa and ~10%, respectively, after the scCO2 treatment and impregnation. The extent of this decrease depended on the supercritical operational parameters. Therefore, filaments with higher antioxidant activity and different expansion degrees and mechanical properties were obtained by adjusting the supercritical processing conditions. [ABSTRACT FROM AUTHOR]

The leaves of Olea europaea as agricultural waste represent a convenient source of antioxidants. In combination with supercritical CO2 (scCO2), assisted impregnation is an interesting strategy for the preparation of biomedical devices with specific bioactivity. For this purpose, 3D-printable filaments of thermoplastic polyurethane (TPU) and polylactic acid (PLA) were employed for the supercritical impregnation of ethanolic olive leaves extract (OLE) for biomedical application. The extraction of OLE was performed using pressurized liquids. The effect of pressure (100–400 bar), temperature (35–55 °C), and the polymer type on the OLE impregnation and the swelling degree were studied including a morphological analysis and the measurement of the final antioxidant activity. All the studied variables as well as their interactions showed significant effects on the OLE loading. Higher temperatures favored the OLE loading while the pressure presented opposite effects at values higher than 250 bar. Thus, the highest OLE loadings were achieved at 250 bar and 55 °C for both polymers. However, TPU showed c.a. 4 times higher OLE loading and antioxidant activity in comparison with PLA at the optimal conditions. To the best of our knowledge, this is the first report using TPU for the supercritical impregnation of a natural extract with bioactivity. [ABSTRACT FROM AUTHOR]