Polymer architecture can be used as a powerful tool for the refinement of materials structure and properties without changing the chemistry of the monomer building blocks. We have used branched copolymers with a bottlebrush architecture to construct various nanostructured materials by covalent and non-covalent assembly. Due to bidirectional nature of the bottlebrush architecture, we probed backbone and side chain asymmetries, as well as side chain arrangement along the backbone as molecular parameters affecting the polymer assembly in dilute solutions and in melts. Aqueous self-assembly of amphiphilic bottlebrush copolymers was used to investigate the effect of structural asymmetry on molecular packing. Interfacial curvature was dictated by the side chain asymmetry, while backbone length was shown to play minimal role in governing the packing of densely grafted bottlebrush apmphiphiles. Molecular packing inside the micellar cores was probed by hydrophobic cargo loading and core cross-linking by strategically placed coumarin functionalities. Tapered bottlebrush copolymers, prepared by one-shot polymerization of macromonomers with vastly different reactivities, boasted a gradient transition of side chain composition between the two blocks. Such interfacial manipulation had a profound effect on polymer self-assembly, offering a new avenue for morphological control.

Bottlebrush copolymers: Morphological control through molecular architecture

255th National Meeting (2018)

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