We report on the preparation of reinforced membranes (SPP-QP-PE, where SPP stands for sulfonated polyphenylene), composed of an in-house proton-conductive polyphenylene ionomer (SPP-QP) and a flexible porous polyethylene (PE) mechanical support layer. By applying the push coating method, dense, uniform, transparent, and thin SPP-QP-PE membranes were obtainable. The use of SPP-QP with higher ion exchange capacity induced very high proton conductivity of SPP-QP-PE, leading to high fuel cell performance even at low humidified conditions (e.g., at 80 °C and 30% relative humidity), which had not been attainable with the existing reinforced aromatic ionomer membranes. The flexible porous PE substrate improved the mechanical toughness of the membranes; the elongation at break increased by a factor of 7.1 for SPP-QP-PE compared to that with the bare SPP-QP membrane, leading to mechanical durability at least 3850 wet-dry cycles under practical fuel cell operating conditions (the United States Department of Energy protocol). Overall, the reinforced aromatic ionomer membranes, SPP-QP-PE with balanced proton conductivity, mechanical toughness, and gas impermeability, functioned well in fuel cells with high performance and durability.
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