Poly(vinylpyridine) chemistry was employed to enhance the chemical tunability, architectural control, and stimuli-responsiveness of covalently crosslinked polymeric materials referred to as macromolecular grafted-through networks (MaGNets). MaGNets bearing poly(vinylpyridine) side groups between poly(exo-norbornene) crosslinks were synthesized using a multi-step, multi-scale approach which included ring-opening metathesis polymerization (ROMP) and reversible addition-fragmentation chain transfer (RAFT). By changing the degree of polymerization of RAFT and/or ROMP, a range of accessible moduli were observed as evidenced by rheological characterization. Network precursors, or macroscale crosslinkers, were synthesized with controllable molecular weights and narrow dispersity values. Having established fundamental structure-property correlations as related to RAFT and ROMP parameters, guest molecules (organic and inorganic) were then introduced into MaGNets and were found to bind to pyridine groups, resulting in tailorable gel properties (modulus, swelling, and stimuli-responsiveness). Finally, networks were synthesized and swollen in various solvents (organic, aqueous), which were found to greatly impact network moduli depending on factors such as pH, acid strength, and solvent polarity.

Poly(vinylpyridine) macromolecular gels: Controlling properties and stimuli-responsiveness via network architecture, guest-molecule coordination, and solvent

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

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