Composite electrolytes
comprising a polymer plus Li salt matrix
and embedded fillers have the potential of realizing high lithium-ion
conductivity, good mechanical properties, wide electrochemical operational
window, and stability against metallic lithium, all of which are essential
for the development of high-energy-density all-solid-state lithium-ion
batteries. In this study, a solvent-free approach has been used to
prepare composite electrolytes with tetragonal and cubic phase garnets
synthesized via nebulized spray pyrolysis with polyethylene
oxide (PEO) being the polymer component. Electrochemical impedance
spectroscopy (EIS) is used to examine a series of composites with
different garnets and weight fractions. The results show that with
the increase in the ceramic weight fraction in the composites, ionic
conductivity is reduced and alternative Li-ion transport pathways
become accessible for composites as compared to the filler-free electrolytes.
An attempt is made to understand the ion transport mechanism within
the composites. The role of the chemical and morphological properties
of the ceramic filler in polymer-rich and ceramic-rich composite electrolytes
is explained by studying the blends of nonconducting ceramics with
the Li-conducting polymer, indicating that the intrinsic conductivity
of the ceramic filler significantly contributes to the overall conductive
process in the ceramic-rich systems. Further, the stability of the
garnet/PEO interface is studied via X-ray photoelectron
spectroscopy, and its impact on the lithium-ion transport is studied
using EIS.