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Control of Phase Separation in Polystyrene/Ionic-Liquid Blended Films by Polymer-Brush-Grafted Particles.

Immiscible composite materials with controlled phase-separated structures are important in area ranging from catalysis to battery. We succeeded in controlling the phase-separated structures of immiscible blends of polystyrene (PS) and two ionic-liquids (ILs), namely, N, N-diethyl- N-(2-methoxyethyl)- N-methylammonium bis(trifluoromethylsulfonyl)imide (DEME-TFSI) and 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EMI-TFSI), by adding precisely designed concentrated-polymer-brush-grafted (CPB-grafted) silica nanoparticles (CPB-SiPs) prepared by surface-initiated atom-transfer radical polymerization. We discuss relationships between chemical species and molecular weights of the CPB and the phase-separated structures. When the CPB was composed of a PS homopolymer of an appropriate molecular weight, the IL phase formed a continuous structure and a quasi-solid blended film was successfully fabricated because the CPB-SiPs were adsorbed at the PS/IL interface and prevented macroscopic phase separation. We propose that CPB-SiP adsorption and the fabrication of quasi-solid films are governed by the degree of penetration of the matrix-PS chains into the CPB and deformability of the CPB-SiPs. We found that the DEME-TFSI domain size can be controlled by the CPB-SiP content, and only 1 wt% of the CPB-SiPs was needed to fabricate a quasi-solid film. In addition, we investigated the ionic properties of the quasi-solid PS/DEME-TFSI blended film. Owing to continuous ion channels composed only of DEME-TFSI, the film exhibited an ionic conductivity of 0.1 mS/cm, which is relatively high when compared to previously reported quasi-solid electrolytes. Finally, we demonstrated that an electric double-layer capacitor fabricated using this film as the electrolyte exhibited high charge/discharge cycling stability and reversibility.

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