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The question of if silica nanoparticles can enhance the ionic conductivity ofa polymer electrolyte above its crystallization temperature has remainedunclear for the two decades following the first experiments on these systems.We use Molecular Dynamics simulations to decipher the atomic scale mechanismsaffecting the properties of LiTFSI-poly(ethylene oxide) electrolytes upon theaddition of silica nanoparticles. At any ionic concentration, addingnanoparticles significantly decreases the conductivity. Most of this reductioncan be simply accounted for by the diffusion equation, resulting from the factthat the space occupied by the nanoparticles is made inactive and unable tosustain ionic diffusion. We identify two distinct regimes, above and below aconcentration threshold, corresponding to very different ionic distributionsand coordination features of the various species. The lack of conductivityenhancement observed in the simulations supports the conclusions of some recentmeasurements, and disagrees with the earliest experimental reports on hybridsilica/polyethylene-oxide electrolytes.

Can silica nanoparticles improve lithium transport in polymer electrolytes?