The Effect of Solvents Dielectric Constant in the Phase Behavior of Complex Coacervation in Polymerized Ionic Liquids (PILs)
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Complex coacervation is notable for its sensitivity to external stimuli, thermodynamic reversibility, and simple processibility. It is driven by entropy gain by counterion release, electrostatic interaction, and polymer-solvent interaction. Although ε_r of solvents indicates the strength of electrostatic interaction and different solvents induce different polymer-solvent interaction, research on solvent effects in complex coacervation has been limited due to the poor solubilities in non-aqueous solvents. We designed two similarly structured PILs to dissolve in various organic solvents with ε_r from 16 to 109. Findings reveals that solvents with similar qualities show similar phase behavior despite their different ε_r. Conversely, solvents with similar ε_r but better qualities exhibit lower stability of complex coacervates, suggesting that the phase behavior of PILs is primarily determined by entropy gain and polymer-solvent interactions, with a minor effect from electrostatic interactions.