De- and Re-Structuring of Starch to Control the Melt and Solid State Visco-Elasticity as Method for Getting New Multi Component Compounds with Scalable Properties.

The aim of the article was to design and develop new thermodynamically stable starch-based compounds, with scalable properties, that are melt-processable into finished products by classic or 3D printing methods. This is based on phenomena of de-structuring, entanglement compatibilization, and re-structuring of starch, along with the modification of the polymer, polyvinyl alcohol (PVA), by following an experimental sequence involving pre-treatment and melt compounding in two stages. The new compounds selection was made considering the dependence of viscoelastic properties on formulation and flowing conditions in both the melted and solid states. Starting from starch with 125 °C glass transition and PVA with a T_g at 85 °C, and following the mentioned experimental sequence, new starch-PVA compounds with a high macromolecular miscibility and proven thermodynamic stability for at least 10 years, with glass transitions ranging from -10 °C to 50 °C, optimal processability through both classical melt procedures (extrusion, injection) and 3D printing, as well as good scalability properties, were achieved. The results are connected to the approaches considering the relationship between miscibility and the lifetime of compounds with renewable-based polymer content. By deepening the understanding of the thermodynamic stability features characterizing these compounds, it can be possible to open the way for starch usage in medium-life compositions, not only for short-life applications, as until now.