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Physicochemical properties of bis(fluorosulfonyl)amide anion-based ionic liquids (ILs) adsorbed on solid oxide electrolyte powder of cubic Li 7 La 3 Zr 2 O 12 (LLZ) partially substituted by Mg and Sr were evaluated.In this study, an experimental system that ion does not pass the interface between LLZ and IL was selected by using ILs without lithium salt in order to elucidate the properties of adsorbed ILs layer. We prepared mixtures of LLZ with 1-methyl-1-propylpyrrolidinium bis(fluorosulfonyl)amide and 1-ethyl-3-methylimidazolium bis(fluorosulfonyl)amide of various average IL thickness on LLZ particles by changing the IL volume per LLZ surface area. Evaluation of ionic conductivity and thermal property, and measurement of nuclear magnetic resonance spectra of these samples were performed. The results indicate the existence of an IL adsorption layer on the LLZ surface that shows solid-like behavior.

We evaluated and compared the physical properties of electrolyte solutions consisting of lithium bis(fluorosulfonyl)amide and sulfone solvents (molar ratio = 1 : 3) and their mixtures containing aluminum oxide (α-Al 2 O 3 ) or lithium lanthanum zirconate (LLZ) particles of various particle sizes. Sulfolane (SL), 3-methylsulfolane, and ethyl isopropyl sulfone were evaluated as sulfone solvents for the electrolyte solutions. The phase-change heat, phase-change temperature, and spin-spin relaxation time in nuclear magnetic resonance (NMR) measurements decrease in a mixture of SL electrolyte with a metal oxide, with an apparent average liquid thickness in the order of nm resulting from the SL electrolyte solution. This indicates a decrease in molecular mobility around the particle surface. For the α-Al 2 O 3 system, no substantial changes are observed in the activation energy of ionic conductivity, self-diffusion coefficient of Li + (determined via pulsed-field gradient NMR), or relative cross-peak intensities of Li + and 1 H of SL in the two-dimensional NMR of the mixture. Therefore, despite its low molecular mobility, the SL electrolyte solution at the solid-liquid interface is considered to exhibit an ionic conductivity mechanism similar to that of the bulk electrolyte. It was suggested that LLZ system has a different ionic conduction mechanism than α-Al 2 O 3 system.