Blended biocomposites created from the electrostatic and hydrophobic interactions between polysaccharides and structural proteins exhibit useful and unique properties. However, engineering these biopolymers into applicable forms is challenging due to the coupling of the material’s physicochemical properties to its morphology, and the undertaking that comes with controlling this. In this particular study, numerous properties of the Bombyx mori silk and microcrystalline cellulose biocomposites blended using ionic liquid and regenerated with various coagulation agents were investigated. Specifically, the relationship between the composition of polysaccharide-protein bio-electrolyte membranes and the resulting morphology and ionic conductivity is explored using numerous characterization techniques, including scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), thermal gravimetric analysis (TGA), differential scanning calorimetry (DSC), X-ray scattering, atomic force microscopy (AFM) based nanoindentation, and dielectric relaxation spectroscopy (DRS). The results revealed that when silk is the dominating component in the biocomposite, the ionic conductivity is higher, which also correlates with higher β-sheet content. However, when cellulose becomes the dominating component in the biocomposite, this relationship is not observed; instead, cellulose semicrystallinity and mechanical properties dominate the ionic conduction.

Electrospinning is a widely used technique to draw recalcitrant biopolymer solutions into micro to nanoscale materials in a simple and economical way. The first focus of this research involved using ionic liquids as a non-volatile solvent for natural insoluble biopolymers such as silk and cellulose (or cellulose derivatives). Compared to traditional organic solvents, ionic liquids can dissolve biopolymers without altering the molecular weight of the biopolymer. In this study, 1-ethyl-3-methylimidizolium acetate (EMIMAc) ionic liquid was used and the regenerated films were coagulated in baths of EtOH or water. The second focus of this research explored the dissolution of IL-regenerated composites into organic solvents and their electrospun composite nanomaterials. Various ratios of silk-cellulose bio-composite films regenerated from ionic liquids were used as the raw materials and sequentially dissolved/dispersed into a Formic Acid-CaCl₂ solution in order to initiate the electrospinning of silk-cellulose nanomaterials. Because of the variability of ionic liquids, the nanomaterials produced using this technique have unique and tunable properties such as large surface area to volume ratios and low structural defects. FTIR and SEM results suggest that the structure and morphology of the final nanosized samples becomes more globular when the biopolymer composition ratio has increased cellulose content. TGA results demonstrated that the electrospun materials have better thermal stability than the original films. This two-step electrospinning method, using ionic liquid as a non-volatile solvent to first dissolve and mix raw natural materials, may lead to extensive research into its biomedical and pharmaceutical applications in the future.