Chitosan (CS) is a polymer extensively used in drug delivery formulations mainly due to its biocompatibility and low toxicity. In the present study, chitosan was used for nanoencapsulation of a budesonide (BUD) drug via the well-established ionic gelation technique and a slight modification of it, using also poly(vinyl alcohol) (PVA) as a surfactant. Scanning electron microscopy (SEM) micrographs revealed that spherical nanoparticles were successfully prepared with average sizes range between 363 and 543 nm, as were measured by dynamic light scattering (DLS), while zeta potential verified their positive charged surface. X-ray diffraction (XRD) patterns revealed that BUD was encapsulated in crystalline state in nanoparticles but with a lower degree of crystallinity than the neat drug, which was also proven by differential scanning calorimetry (DSC) and melting peak measurements. This could be attributed to interactions that take place between BUD and CS, which were revealed by FTIR and by an extended computational study. An in vitro release study of budesonide showed a slight enhancement in the BUD dissolution profile, compared to the neat drug. However, drug release was substantially increased by introducing PVA during the nanoencapsulation procedure, which is attributed to the higher amorphization of BUD on these nanoparticles. The release curves were analyzed using a diffusion model that allows estimation of BUD diffusivity in the nanoparticles.
Despite the advantages of polylactide (PLA), its inadequate UV-shielding and gas-barrier properties undermine its wide application as a flexible packaging film for perishable items. These issues are addressed in this work by investigating the properties of melt-mixed, fully bioderived blends of polylactide (PLA) and poly(ethylene furanoate) (PEF), as a function of the PEF weight fraction (1–30 wt %) and the amount of the commercial compatibilizer/chain extender Joncryl ADR 4468 (J, 0.25–1 phr). J mitigates the immiscibility of the two polymer phases by decreasing and homogenizing the PEF domain size; for the blend containing 10 wt % of PEF, the PEF domain size drops from 0.67 ± 0.46 µm of the uncompatibilized blend to 0.26 ± 0.14 with 1 phr of J. Moreover, the increase in the complex viscosity of PLA and PLA/PEF blends with the J content evidences the effectiveness of J as a chain extender. This dual positive contribution of J is reflected in the mechanical properties of PLA/PEF blends. Whereas the uncompatibilized blend with 10 wt % of PEF shows lower mechanical performance than neat PLA, all the compatibilized blends show higher tensile strength and strain at break, while retaining their high elastic moduli. The effects of PEF on the UV- and oxygen-barrier properties of PLA are also remarkable. Adding only 1 wt % of PEF makes the blend an excellent barrier for UV rays, with the transmittance at 320 nm dropping from 52.8% of neat PLA to 0.4% of the sample with 1 wt % PEF, while keeping good transparency in the visible region. PEF is also responsible for a sensible decrease in the oxygen transmission rate, which decreases from 189 cc/m2·day for neat PLA to 144 cc/m2·day with only 1 wt % of PEF. This work emphasizes the synergistic effects of PEF and J in enhancing the thermal, mechanical, UV-shielding, and gas-barrier properties of PLA, which results in bioderived blends that are very promising for packaging applications.
Vanillic acid that can be prepared from lignin through vanillin is a relatively new and most promising aromatic monomer for the synthesis of biobased polyesters. Due to its structural similarity to terephthalic acid, vanillic acid-containing polymers have been reported to exhibit comparable properties to poly(ethylene terephthalate). Herein, the nanomechanical and thermal properties and crystallization behavior of poly(propylene vanillate) (PPV), a new alipharomatic biobased polyester synthesized from 4-(2-hydroxypropoxy)-3-methoxybenzoic acid, are reported. As the phase transitions dominate the processing of polymers and determine the processing temperature window, the melting, crystallization, and glass transition temperatures were determined, and the thermodynamics and kinetics of phase changes were studied. The enthalpy of fusion was estimated (ΔH m 0 = 162 J/g), and the equilibrium melting temperature (T m 0 = 220.5 °C) was calculated using the Hoffman−Weeks method. The multiple melting behavior of PPV was interpreted based on the melting-recrystallization model. Isothermal crystallization was studied. Since processing is always dynamic in industries, the non-isothermal crystallization profiles from the melt or from glass were investigated; differential scanning calorimetry (DSC), wide-angle X-ray diffraction (WAXD), and polarized light microscopy (PLM) were elaborated. Finally, as the mechanical properties of aromatic polymers are of crucial importance for applications, the mechanical behavior of amorphous and annealed PPV samples was examined via nanoindentation.
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