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High-Modulus, High-Conductivity Nanostructured Polymer Electrolyte Membranes via Polymerization-Induced Phase Separation

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journal contribution
posted on 08.01.2014, 00:00 by Morgan W. Schulze, Lucas D. McIntosh, Marc A. Hillmyer, Timothy P. Lodge
The primary challenge in solid-state polymer electrolyte membranes (PEMs) is to enhance properties, such as modulus, toughness, and high temperature stability, without sacrificing ionic conductivity. We report a remarkably facile one-pot synthetic strategy based on polymerization-induced phase separation (PIPS) to generate nanostructured PEMs that exhibit an unprecedented combination of high modulus and ionic conductivity. Simple heating of a poly­(ethylene oxide) macromolecular chain transfer agent dissolved in a mixture of ionic liquid, styrene and divinylbenzene, leads to a bicontinuous PEM comprising interpenetrating nanodomains of highly cross-linked polystyrene and poly­(ethylene oxide)/ionic liquid. Ionic conductivities higher than the 1 mS/cm benchmark were achieved in samples with an elastic modulus approaching 1 GPa at room temperature. Crucially, these samples are robust solids above 100 °C, where the conductivity is significantly higher. This strategy holds tremendous potential to advance lithium-ion battery technology by enabling the use of lithium metal anodes or to serve as membranes in high-temperature fuel cells.

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