Characterization of thin film Li0.5La0.5Ti1-xAlxO3 electrolyte for all-solid-state Li-ion batteries

Abstract

Since addition of Al in Li0.5La0.5TiO3 has enhanced ionic conductivity in bulk materials, it is important to apply this material on all solid state thin film batteries. Because some of the good ionic conductors such as Lithium Phosphorus Oxynitride (LiPON) are sensitive to oxygen and moisture and their application is limited, so amorphous Li0.5La0.5Ti1−xAlxO3 (LLTAlO) is a most promising candidate because of its stability. In this study, the crystalline LLTAlO targets were prepared changing the amount of x content by conventional solid state reactions. Using these targets, lithium lanthanum titanium oxide (LLTO) thin film electrolytes were deposited on ITO/SLG substrates by radio frequency magnetron sputtering system in Ar atmosphere. The structural and compositional properties of targets and thin films were characterized by SEM, XRD, Raman spectroscopy and XPS. It was found that all targets are crystalline while the thin films are amorphous. To understand the effect of Al doping on ionic conductivity, electrical measurements were done at room temperature by AC impedance spectroscopy forming ITO/LLTAlO/Al structure like capacitor. Highest ionic conductivity result, 0.96 × 10−6 S·cm−1, is obtained from the nominal thin film composition of Li0.5La0.5Ti1−xAlxO3 (x = 0.05) at room temperature measurements. Heat treatment is also conducted to investigate to understand its effect on ionic conductivity and the structure of the thin films. It is found that ionic conductivity enhances with annealing. Also, temperature dependent ionic conductivity measurements from 298 K to 385 K are taken in order to evaluate activation energy for Li-ion conduction.