Enhancement in Li-ion Conductivity through Co-doping of Ge and Ta in Garnet Li$_7$La$_3$Zr$_2$O$_{12}$ Solid Electrolyte

TL;DR

This study enhances Li-ion conductivity in garnet solid electrolytes by co-doping with Ge and Ta, achieving high ionic conductivity and stability suitable for solid-state batteries.

Contribution

It introduces a co-doping strategy with Ge and Ta in garnet Li$_7$La$_3$Zr$_2$O$_{12}$ to significantly improve ionic conductivity for battery applications.

Findings

Maximum ionic conductivity of 6.61 x 10$^{-4}$ S/cm at 25°C.

Optimal doping level is 0.25 Ta with activation energy 0.25 eV.

Ceramic stability maintained after 5 months exposure.

Abstract

For being used as an electrolyte in All Solid State Batteries (ASSB), a solid electrolyte must possess ionic conductivity comparable to that of conventional liquid electrolytes. To achieve this conductivity range, the series Li$_{6.8-y}$Ge$_{0.05}$La$_3$Zr$_{2-y}$Ta$_y$O$_{12}$ ($y = 0, 0.15, 0.25, 0.35, 0.45$) has been synthesized using solid-state reaction method and studied using various characterization techniques. The highly conducting cubic phase is confirmed from XRD analysis. Structural information was collected using SEM and density measurements. The prepared ceramic sample containing 0.25 Ta, sintered at 1050$^\circ$C for 7.30 hrs shows the maximum ionic conductivity of 6.61 x 10$^{-4}$ S/cm at 25$^\circ$C. The air stability of the same ceramic has also been evaluated after exposure for 5 months. The minimum activation energy associated with the maximum conductivity of 0.25 Ta is 0.25 eV. The DC conductivity measurements were done to confirm the ionic nature of conductivity for all ceramic samples. The stable result of ionic conductivity makes the 0.25 Ta containing ceramic sample a promising candidate for solid electrolytes for ASSB applications.