Soggy-sand electrolytes (solid-liquid composites, typically gel electrolytes, with synergistic electrical properties) are reviewed as far as status and perspectives are concerned. Major emphasis is put on the understanding of the local mechanism as well as the long-range transport along the filler network. The beneficial property spectrum includes enhanced conductivity of one ion type and decreased conductivity of the counter ion, but also the exciting mechanical properties of the solid-liquid composites. Inherent but not insurmountable problems lie in the reproducibility and stationarity of the composites microstructure and morphology. Owing to the huge parameter complexity and hence to the multitude of adjusting screws, there are various strategies for materials optimization. The technological relevance is enormous, in particular for battery electrolytes as here all the above-mentioned electrical and mechanical benefits are welcome. The soggy-sand electrolytes combine high Li(+) conductivity, low anion conductivity and good wettability of electrode particles with the mechanical stability of semi-solids.
Using the example of SiO 2 dispersions in LiClO 4 /polyethylene glycol electrolytes, the conduction mechanism of "soggy sand" electrolytes is discussed. The study is essentially based on zeta potential, impedance and transference number measurements as well as on modeling. All the results can be explained by anion adsorption by the oxide particles and increased concentration of free Li + in the double layer. The initially colloidal dispersion quickly forms fractal networks by cluster-cluster aggregation. Once they percolate, an interfacially dominated Li + conductance is observed. The subsequent coarsening of the network is self-decelerating leading to a steady state conductivity that is, for low volume fractions, enhanced compared to SiO 2 free electrolytes. At higher values, blocking and inhomogeneity effects (e.g., salt trapping) lead to decreased values of the overall conductivity.
The formation of fractal silica networks from a colloidal initial state was followed in situ by ion conductivity measurements. The underlying effect is a high interfacial lithium ion conductivity arising when silica particles are brought into contact with Li salt-containing liquid electrolytes. The experimental results were modeled using Monte Carlo simulations and tested using confocal fluorescence laser microscopy and ζ-potential measurements.
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