Peptide-Based Context-Adaptive Supramolecular Networks

Peptides have tremendous potential as building blocks of designer materials with wide-ranging applications. These materials are stabilized by strongly directional hydrogen bonding patterns giving rise to one-, or two-dimensional assembly. It remains a challenge to mimic biology’s context-adaptive and flexible structures. In this talk we introduce minimalistic di- and tripeptide sequences that form dynamic ensembles through incorporation of multivalent sidechain interactions that collectively self-optimize depending on their context. We explore the di- and tripeptide sequence spaces to establish design rules for formation of supramolecular dispersions. We demonstrate that these dispersions can display supramolecular recognition of small molecules, including sugars. Notably, we observed that these supramolecular dispersions undergo drying-induced liquid to solid phase separation involving interface stabilization and expansion, resulting in formation of films of stiff, and densely packed, porous peptide microparticles that can be instantaneously redispersed upon re-introduction of water. Air-drying of aqueous peptide dispersions in the presence of proteins or small molecule payloads results in spontaneous and efficient encapsulation, and retention of protein stability after redispersion. These supramolecular tripeptide dispersions therefore show promise for recognition, emulsification, encapsulation, and storage of biomacromolecules.