Supramolecular self-assembly offers access to tough, stimuli-responsive materials through the careful design of non-covalent interactions. The contribution of these interactions to bulk material behavior, e.g. mechanical toughness, is dictated by the interaction type, self-assembled architecture, and environment surrounding the supramolecular motifs. Metal-ligand coordination interactions offer a convenient platform for introducing thermo- and chemoresponsive properties into a self-assembled network, striking a balance between strong interactions and responsiveness. In this work, we focus on the incorporation of metal-coordination supramolecular interactions into covalently-crosslinked elastomers as a platform for tuning self-assembly in supramolecular polymer networks. Orthogonal incorporation of a covalently crosslinked network and supramolecular polymer results in a semi-interpenetrating network (SIPN). Using this strategy, manipulating the covalently crosslinked environment around the supramolecular polymer offers control over microphase separation, material mechanics, and stimuli-responsive behavior. Via this SIPN framework, changes in interfacial area as the morphology shifts from droplets-in-a-matrix to co-continuous are shown to dictate supramolecular ordering and shift bulk deformation response through both the disruption of self-assembly and changes in crack propagation behavior. Extending this work, we explore how supramolecular ordering dictates stimuli-responsive behavior, such as the dissociation of non-covalent motifs, and bulk mechanics in self-assembled elastomer networks for applications in areas such as shape memory and sensing.

Impact of non-covalent ordering on mechanics and stimuli-responsive behavior in supramolecular polymer networks

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.