Rationally designed mucin-like glyco and peptide hydrogels

The two systems are based on a scaffold (either a coiled-coil peptide or a self-assembling oligosaccharide) substituted with carbohydrate units. For each system, we explored synthesis, assembly process, and rheological properties.

Peptide-based hydrogels: Coiled-coil peptides were functionalized with synthetic glycans to generate a library of glycopeptides. We constructed an atomistic model of the peptide-based scaffold and simulated the assembly process. The simulations and rheological experiments showed that a chromophore label at the end of coiled-coil peptide dimers modifies the hydrogen-bond patterns at the coiled-coil interface and thereby controls the viscoelastic properties of the hydrogel. The hydrogels were analyzed with nano, micro and macro rheology revealing that small differences in the carbohydrate structure have a substantial effect on the properties of the hydrogel (A02|Gradzielski/Netz, A04|Seitz/Block).

Carbohydrate-based hydrogels: We discovered that cellulose oligomers substituted with different carbohydrate units at the termini assemble into supramolecular hydrogels. These gels were characterized with a variety of microscopy techniques (Z01|Mertins/Ludwig/Pigaleva), confirming the formation of cellulose-based assemblies with a dense presentation of different glycans on their surface. These self-healing hydrogels showed rheological properties in the same range of native mucus, but allowed for full control over molecular composition.