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Partial Solvation of Lithium Ions Enhances Conductivity in a Nanophase-Separated Polymer Electrolyte

Vigil, Daniel L.; Frischknecht, Amalie L.; Stevens, Mark J.; Winey, Karen I.; Ferko, Benjamin T.; Mecking, Stefan; Saumer, Anne

In this study, we demonstrate that a multiblock lithium-ion-conducting polymer can be swollen with ethylene carbonate solvent to increase the conductivity relative to the dry polymer material by nearly 4 orders of magnitude. This increase is due to the partial solvation of lithium ions by ethylene carbonate, which leads to Li+ diffusion along the solvent–polymer interface. This differs from the vehicular transport mechanism for lithium ions in pure solvent. We use a combination of broadband dielectric spectroscopy, X-ray scattering, and all-atom molecular dynamics simulations to probe the effect of the solvent on the polymer morphology and to elucidate the mechanism of lithium ion transport.

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