Unsaturated vegetable oils with conjugated carbon–carbon double bonds, such as tung oil, can undergo free-radical polymerization, originating alternatives to petroleum-based materials. The introduction of fillers to vegetable oil-based polymer matrices results in composites with improved mechanical properties. In this work, thermosets were synthesized by the free-radical polymerization of a mixture of tung oil, divinylbenzene, and n-butyl methacrylate, and reinforced with bio-based fillers, namely Miscanthus, Pinus taeda (also known as southern pine), and algae (Microspora and Oedogonium) biomass. The effect of filler particle size on the composites’ properties was evaluated. Additionally, to develop a better interaction between the hydrophobic resin and the hydrophilic reinforcements, and improve the mechanical properties of the composites prepared, itaconic anhydride, a bio-based molecule derived from itaconic acid, was added to the resin. Thermogravimetric analysis (TGA) showed that the presence of itaconic anhydride improved the overall thermal stability of the composites. The storage modulus of the composites at room temperature, assessed by dynamic mechanical analysis (DMA), was increased by approximately 32% and 68%, for Miscanthus and southern pine composites, respectively, when itaconic acid was added to the resin. It was also observed that the glass transition temperatures were not significantly affected by the presence of itaconic acid. Scanning electron microscope (SEM) images indicated better matrix-reinforcement adhesion in the presence of itaconic anhydride.
Sustainable and renewable polymeric materials are gaining traction, and vegetable oils have been used directly or in modified forms to meet this demand. At the same time, microbial hosts (such as the oleaginous yeast Yarrowia lipolytica) are being touted as sustainable alternatives for petroleum and vegetable oils. However, the exact role of fatty acid composition and speciation on polymer performance remains unclear. Here, we explore a datadriven approach to explicitly relate the underlying oil composition with the thermomechanical properties of the resulting polymeric material. In doing so, we identify the C16:0, C16:1, and C18:0 fatty acid contents of vegetable oils as critical parameters for predicting thermal stability at maximum heat loss (T max ). Machine learning-based approaches were applied to study the link between thermal properties and monomer composition. In the end, application of multiple linear regression modeling indicated strong dependence on the C16:1 content as evident by the parameter loading (loading of +428 for T max ). As a more sustainable source of oil, Y. lipolytica oil-based polymer properties were also dictated by the C16:0 and C18:0 fatty acid contents but with an opposite impact as compared with vegetable oils (T max loadings of −208 and +36 for Y. lipolytica oils, +19 and −72 for vegetable oils, C16:0 and C18:0, respectively). Despite these differences, Y. lipolytica oilbased polymers showed similar strength and cross-linking density to vegetable oil polymers. This work is the first evaluation of polymer properties from a library of vegetable-and yeast-sourced oils and highlights a mechanistic understanding of thermal stability from both oil source (vegetable or microbial) and oil composition that can be used for future design.
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