Enhancement of density and ionic conductivity for garnet-type Li5La3Ta2O12 solid electrolyte by self-consolidation strategy

Garnet-type Li₅La₃Ta₂O₁₂ (LLTaO) solid electrolyte is a potential candidate component for future all-solid-state batteries due to its extraordinary stability against the reaction with molten lithium. In contrast with traditional cold isostatic pressing (CIP) method, which generally pursues ultra-high pressure, this paper tries to enhance the density and ionic conductivity of LLTaO by self-consolidation strategy without the assistance of any pressing operations. A LLTaO bulk with a relative density of 95% is obtained. SEM images reveal that the bulk sample is assembled by large dense particles in size of tens of microns indicating that the interstitial space among the particles has been dramatically minimized. Accordingly, the total ionic conductivity and the bulk ionic conductivity at 30?°C are promoted up about one order of magnitude higher to 2.63?× 10^?5 S?cm^?1 and 1.41?×?10^?4 S?cm^?1, respectively. Moreover, the lithium ionic migration network in the crystalline unit cell of LLTaO is first explored from its assembled way. A hexagon-like basic unit with tetrahedral Li1 joint sites and Li1- - Li1 edges is identified. The tetrahedral Li1 sites act as crucial junctions for the transportation of lithium ions. This work would significantly stimulate the development of LLTaO electrolyte membrane technology.