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Preparation of highly proton-conductive and thermoplastic composites was successfully pursued from H3PO4-doped silica gel and organic polymers with sulfo groups. The sulfo groups and polystyrene blocks in the organic polymers were found to improve the proton conductivity and molding characteristics of the resultant composite, respectively. The composite composed of H3PO4-doped silica gel with a molar ratio=0.5 of H3PO4/SiO2 in 80mass% and sulfonated styrene-isoprene-styrene (SIS-SO3H) block copolymer in 20 mass% showed a high electrical conductivity of 10-4S·cm-1 at 25°C in dry N2 atmosphere and good molding characteristics. The temperature dependence of the electrical conductivity of the composite was of the Vogel-Tamman-Fulcher type, indicating that proton transferred through a liquid-like phase present in the composites consisting of silica gel and organic polymer. The elastic modulus of the composite was larger by one to two orders of magnitude than that of the SIS-SO3H elastomer. The thermoplastically deforming temperature of the composite was around 130°C, which was higher by 50°C than that of the SIS elastomer itself. The capacitance of a totally solid state electric double-layer capacitor, which was fabricated using the composite as a solid electrolyte, was comparable to those of the conventional capacitors with liquid electrolytes.

Proton-Conductive Composites Composed of Phosphoric Acid-Doped Silica Gel and Organic Polymers with Sulfo Groups.