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We report on a novel approach to synthesize cubic-phase fast ionic conductinggarnet-type solid state electrolytes based on Bi doped Li7La3Zr2O12 (LLZO). Bialiovalent substitution into LLZO utilizing the Pechini processing method issuccessfully employed to synthesize Li7-xLa3Zr2-xBixO12 compounds. Ionicconductivities up to 2.0 x 10-4 S/cm are achieved in structures not fullydensified. Cubic phase Li6La3ZrBiO12 powders are generated in the temperaturerange from 650 {\deg}C to 900 {\deg}C in air. In contrast, in the absence of Biand under identical synthesis conditions, the cubic garnet phase ofLi7La3Zr2O12 is not formed below 700 {\deg}C while a transformation to thetetragonal phase is observed at 900 {\deg}C for the un-doped compound. Thecritical role of Bi in lowering the formation temperature of the garnet cubicphase and the improvements in ionic conductivity is investigated in this workthrough microstructural studies and AC impedance measurements. We ascribe theeffect of Bi doping in achieving these remarkable improvements to significantenhancements at lower temperatures in the kinetics of the solid-state reactionresulting in explosive grain growth and densification of the garnet. Moreover,XAS is utilized to identify the specific atomic site where Bi is incorporatedin the LLZO garnet crystalline structure.

Ionic conductivity enhacements and low temperature synthesis of Li7La3Zr2O12 garnets by Bi aliovalent substitutions