The new trend in food packaging films is to use biodegradable or bio-based polymers, such as poly(lactic acid), PLA with additives such as thymol, carvacrol, limonene or cinnamaldehyde coming from natural resources (i.e., thyme, oregano, citrus fruits and cinnamon) in order to extent foodstuff shelf-life and improve consumers’ safety. Single, triple and quadruple blends of these active compounds in PLA were prepared and studied using the solvent-casting technique. The successful incorporation of the active ingredients into the polymer matrix was verified by FTIR spectroscopy. XRD and DSC data revealed that the crystallinity of PLA was not significantly affected. However, the Tg of the polymer decreased, verifying the plasticization effect of all additives. Multicomponent mixtures resulted in more intense plasticization. Cinnamaldehyde was found to play a catalytic role in the thermal degradation of PLA shifting curves to slightly lower temperatures. Release of thymol or carvacrol from the composites takes place at low rates at temperatures below 100 °C. A combined diffusion-model was found to simulate the experimental release profiles very well. Higher antioxidant activity was noticed when carvacrol was added, followed by thymol and then cinnamaldehyde and limonene. From the triple-component composites, higher antioxidant activity measured in the materials with thymol, carvacrol and cinnamaldehyde.
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