Bottlebrush polymers, macromolecules consisting of dense polymer brushes grafted from a central polymer backbone, demonstrate unique physical and material properties resulting from their architecture. With the advent of controlled radical polymerization techniques, access to these macromolecular architectures has become readily available. However, synthetic challenges remain including the need for intermediate purification steps, the use of toxic solvents, and challenges with achieving large bottlebrushes as a result of backbone entanglements. In this work we report on a strategy to prepare hybrid bonding bottlebrush polymers consisting of water soluble poly(sodium 4-styrenesulfonate) brushes grafted from a peptide amphiphile supramolecular polymer backbone. This was achieved through photo-initiated reversible addition-fragmentation chain transfer polymerization in an aqueous environment using a photocatalyst and mild visible light. The rheological properties of the bottlebrush polymers were assessed, with the hybrid bottlebrush providing enhanced solution viscosity, and with appropriate grafting densities, self-healing capabilities when compared to controls. Finally, a proteoglycan mimetic hybrid bottlebrush polymer was synthesized, and the effect this unique architecture has on stem cell fate investigated. Taken together, our results indicate great opportunity for hybrid bonding bottlebrush polymers given their ease of synthesis, self-healing viscoelastic properties, and suitability for biomedical applications.

Peptide amphiphile based hybrid bonding bottlebrush polymers

ACS Spring 2022

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