(Invited) Beyond Dendrites, Cycling Li-Metal across Garnet at High Current Densities

Abstract

Solid-state Li-batteries (SSLiBs) have the potential to be a transformational and intrinsically safe energy storage solution. However, their progress has been limited by high solid-solid interfacial impedance and numerous reports of Li-dendrites and a corresponding “critical current density”. By first modifying the garnet surface to enable Li-metal to wet it and then fabricating garnet-electrolytes into tailored tri-layer microstructuresto form electrode supported dense thin-film (~10μm) solid-state electrolytes we have been able to overcome these limitations. The microstrucurally tailored porous garnet scaffold support increases electrode/electrolyte interfacial area, overcoming the high impedance typical of planar geometry SSLiBs resulting in an area specific resistance (ASR) of only ~2 to 7 Ωcm-2at room temperature. The unique garnet scaffold/electrolyte/scaffold structure further allows for charge/discharge of the Li-metal anode and cathode scaffolds by pore-filling, thus providing high depth of discharge ability without mechanical cycling fatigue seen with typical electrodes. Moreover, these scalable multilayer ceramic fabrication techniques, without need for dry rooms or vacuum equipment, provide for dramatically reduced manufacturing cost. The fabrication of supported dense thin-film garnet electrolytes, their ability to cycle Li-metal at high current densities with no dendrite formation, and results for Li-metal anode/garnet-electrolyte based batteries with a number of different cathode chemistries will be presented.