Optimization of Lithium Content and Sintering Aid for Maximized Li+ Conductivity and Density in Ta-Doped Li7La3Zr2O12

Ta-doped cubic phase Li7La3Zr2O12 (LLZ) lithium garnet received considerable attention in recent times as prospective electrolyte for all-solid-state lithium battery. Although the conductivity has been improved by stabilizing the cubic phase with the Ta5+ doping for Zr4+ in LLZ, the density of the pellet was found to be relatively poor with large amount of pores. In addition to the high Li+ conductivity, density is also an essential parameter for the successful application of LLZ as solid electrolyte membrane in all-solid-state lithium battery. Systematic investigations carried out through this work indicated that the optimal Li concentration of 6.4 (i.e., Li6.4La3Zr1.4Ta0.6O12) is required to obtain phase pure, relatively dense and high Li+ conductive cubic phase in Li7-xLa3Zr2-xTaxO12 solid solutions. Effort has been also made in this work to enhance the density and Li+ conductivity of Li6.4La3Zr1.4Ta0.6O12 further through the Li4SiO4 addition. A maximized room-temperature (33 degrees C) total (bulk+grain boundary) Li+ conductivity of 3.7x10(-4)S/cm and maximized relative density of 94% was observed for Li6.4La3Zr1.4Ta0.6O12 added with 1wt% of Li4SiO4.