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Ion-pair comonomers (IPCs) where both the anion and cation contain polymerizable functional groups offer a route to prepare polyampholyte, ion-containing polymers. Polymerizing vinyl functional groups by free-radical polymerization produces bridging ion-pairs that act as non-covalent crosslinks between backbone segments. In particular the homopolymerization of the IPC vinyl benzyl tri -n- octylphosphonium styrene sulfonate produces a stiff, glassy polymer with a glass transition temperature ( T g  ) of 191 °C, while copolymerization with a non-ionic acrylate produces microphase separates ionomers with ion-rich and ion-poor domains. This work investigates the tuning of the  T g   of the polyelectrolyte or ion-rich domains of the ionomers by copolymerizing with vinyl benzyl tri -n- octylphosphonium  p- toluene sulfonic acid. This chemically similar repeat unit with pendant rather than bridging ion-pairs lowers the  T g   compared to the polyelectrolyte or ionomer containing only the IPC segments. Rheological measurements were used to characterize the thermomechanical behavior and  T g   of different copolymers. The  T g   variation in the polyelectrolyte vs. weight fraction IPC could be fit with either the Gordon–Taylor or Couchman–Karasz equation. Copolymerization of IPC with a chemically similar cationic monomer offers a viable route to systematically vary the  T g   of the resulting polymers useful for tailoring the material properties in applications such as elastomers or shape memory polymers.

gels

Systematic Modification of the Glass Transition Temperature of Ion-Pair Comonomer Based Polyelectrolytes and Ionomers by Copolymerization with a Chemically Similar Cationic Monomer