Natural Blends of Ethyl Cellulose Oleogels for Tunable Bioplastic Design

Recently, ethyl cellulose Oleogels have been proposed as gel state, biobased, and biodegradable thermoplastics. This study explores new Oleogel formulations by tailoring the oil phase to improve material customizability. Four classes of biobased oily molecules were selected: a hydroxylated triglyceridecastor oil, a free fatty acidoleic acid, a phenolic lipidcardanol, and a citric acid derivativetributyl citrate. These formulations allowed us to assess the influence of each molecule on the chemical, physical, and mechanical properties of the Oleogels. Cardanol provided the most effective plasticization, increasing elongation at break by 5.6-fold, while oleic acid induced the largest reduction in glass-transition temperature (Δ<i>T</i> _g ∼ 50 °C). Castor oil, in contrast, achieved a balance between elasticity and stability, preserving the tensile strength and thermal resistance. The study presents a comprehensive rheological, mechanical, and physicochemical characterization of these thermoplastic Oleogels, highlighting their potential as a new class of tunable bioplastics.