- Research Article
2
- 10.1021/acs.macromol.5c01318
Unravelingthe Temperature-Dependent Relaxation Dynamicsof Ionic Liquid-Plasticized Compleximers
- Jul 11, 2025
- Macromolecules
- Sophie G M Van Lange + 7 more +7
Polyelectrolytes with ionic domains screened by bulkyhydrophobicsegments form processable, hydrophobic complexes called “compleximers”.Ionic liquids, which are chemically similar, further plasticize compleximers,yet the mechanisms behind their plasticization effects and distributionwithin the complexes remain unclear. This study examines the relaxationdynamics of plasticized compleximers across multiple length scalesusing rheology, fluorescence recovery after photobleaching (FRAP),and broadband dielectric spectroscopy (BDS). The incorporation ofionic liquids into compleximers reduces their glass transition temperature(Tg), accelerates diffusive processes,increases segmental motion, and leads to a small decrease in activationenergy associated with these relaxation processes. However, the activationenergies vary substantially between techniques, probing differentphysical processes: approximately 200 kJ/mol in rheology, 50 kJ/molin FRAP, and 90 kJ/mol in BDS. These variations suggest that collectivedynamics strongly influence the compleximer rheology, making the mobilization(and activation) of polymer chains distinct from the local movementof ionic segments.
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