Abstract

For the next generation of safe and high energy rechargeable lithium metal batteries, we introduce nanostructured polymer particles of asymmetric miktoarm star copolymers as additives to liquid electrolytes for use as solid polymer electrolytes (SPE). The mechanical properties of the resulting SPEs are dramatically improved compared to the pure liquid electrolyte (the elastic modulus increased by up to 8 orders of magnitude), while the ionic conductivity was maintained close to that of the pure liquid electrolyte. In particular, the addition of 44 wt % miktoarm stars, composed of ion conducting poly(ethylene oxide), PEO, arms that complement stiff insulating polystyrene arms, PS ((PS)n(PEO)n, where n = 30 the number of arms), in a low molecular weight PEO doped with lithium bis(trifluoromethane)sulfonamide (LiTFSI), resulted in SPEs with a shear modulus of G′ ∼ 0.1 GPa and ion conductivity σ ∼ 10–4 S/cm. The SPEs show a strong decoupling between the mechanical behavior and the ionic conductivity as G′ rem...

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