Establishment of Structure-Property-Processing Relationships for Design of Sprayable Hydrogels and Amyloid/PEO Electrospun Composites

The focus of this dissertation is the design, synthesis, characterization, and prototyping of bio-inspired materials to understand the role of structure, intermolecular interactions, and processing technique on the self-assembly, bioactive properties, and mechanical properties of the biomaterials. This work is divided into three research areas: 1) sprayable and adhesive glycopolymer based hydrogels; 2) decapeptide-based composite nanofiber mats; and 3) prototyping sutures and meshes via electrospinning. The established structure-property-processing relationships provide a foundation for designing biomaterials in the future. The first chapter provides an introductory overview of the requirements necessary for the development of hydrogels, glycopolymers, and peptides, including relevant processing techniques and the motivation of this dissertation. The second chapter addresses a common issue (material dripping from traditional hydrogel sprays) that we solved by creating a shear-responsive hydrogel design. This research underscores the intricate relationships among polymer structure, hydrogel characteristics, and spray processing. In the third chapter, two functional amyloid-like decapeptides with unique assembly morphologies were selected for use as property enhancing bio-additives. Various blends of DP/PEO were fabricated into composite mats via electrospinning to determine how peptide sequence, assembly morphology, and loading levels impact the thermal, mechanical, and morphological properties of nanofiber composite mats. This exploration sets the groundwork for designing amyloid-based biomaterials tailored to specific properties. In the fourth chapter, the fabrication workflow of electrospun sutures and meshes was established. In the last chapter, a summary of the conclusions and suggested future work were provided.