Synthesis and properties of glycopolypeptide biohybrid materials Theme: Novel Polymer Synthesis and New Supramolecular Polymer Assemblies

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The field of synthetic polypeptides has seen many significant advances in recent years, including studies on block and hybrid copolypeptides that form vesicles, fibrils, and other structures with potential applications in medicine and materials chemistry. However, the development of glycosylated polypeptides has not kept pace, primarily due to the inability to readily synthesize glycopolypeptides in a controlled manner. Glycosylation of natural proteins provides diverse functionality such as mediation of recognition events, modification of protein conformations, protection from proteases, and lubrication in eyes and joints. Our goal is to prepare glycosylated polypeptides and polysaccharidepolypeptide biohybrids with controlled placement of sugar functionality. We expect these materials will display novel structural and physical properties, and will tune biocompatibility and cell-binding ability when included in core-shell particles, vesicles and hydrogels. Our group combines expertise from four countries in polypeptide synthesis, polymer-analogous reactions, preparation and characterization of self-assembled materials, and evaluation of self-assemblies in cell culture and animal models. We will develop different yet complimentary strategies to prepare glycopeptide polymers, which will allow us to prepare a more diverse range of materials than any of our team could produce separately. Our methods include: controlled polymerization of new glyco-amino acid monomers, azide-alkyne and thiol-ene conjugation of sugars onto polypeptides, and chain-end and side-chain coupling of oligosaccharides and polypeptides. We will work together to combine these methods for preparation of unprecedented block glycopeptides containing multiple types of sugar functionality for use in self-assembling materials. These materials will be characterized to determine how the sugar linkage and placement of sugar functionality along the chain influences physical, structural and biochemical properties. A key advantage of our approach is that complex glycopolymers will be prepared in a rapid and scalable manner, which allows fine tuning of properties through careful adjustment of compositions and architectures.