Coiled-coil peptide units, or bundlemers, have utility as a macromonomeric building block to synthesize complex supramolecular architectures. The bundlemer is a computationally designed monodisperse nanoparticle that exhibits the exact positioning of chemistry at its periphery and is easily modified to incorporate a large array of possible chemical handles. In this work, polymers are grafted from the peptidic backbone of the bundlemer via photoinduced atom transfer radical polymerization (photoATRP), resulting in a supramolecular star copolymer. Specifically, an alkyl halide ATRP initiator is conjugated to the peptide backbone and poly 2-(dimethylamino)ethyl methacrylate (PDMAEMA) is polymerized from the desired position along the bundlemer periphery. We show the successful growth of polymer with conversions around 85% and relatively low dispersities. Additionally, we demonstrate that the bundlemer remains assembled after polymerization and that the resulting conjugate exhibits responsiveness to changes in environmental conditions. These results indicate success in synthesizing a precise, unique, and supramolecular nanostructure with tunable features that can be targeted for specific applications.

Bundlemers as supramolecular building blocks for synthesizing peptide polymer conjugates

ACS Spring 2022

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