Abstract
Li-metal batteries with solid oxide electrolytes have garnered increasing attention as promising technologies that can overcome the safety and energy density limits of lithium-ion batteries (LIBs). However, the less than satisfactory long-term stability of Li-metal batteries-a consequence of Li dendrite formation caused by unstable Li plating/stripping at the interface between the Li metal and solid electrolyte-is hampering their commercialisation. Herein, we propose an negative electrode multilayer consisting of porous Te and carbon-based layers that can suppress Li dendrite formation and significantly lower the degree of capacity decay during long-term cycling. A quasi-all-solid-state Li-metal battery fabricated using Li(6.4)La(3)Zr(1.7)Ta(0.3)O(12) (LLZTO), a Te/Ag-C anodenegative electrode interlayer, and a LiNi(0.8)Co(0.1)Al(0.1)O(2) (NCA811) positive electrode impregnated with an ion-conducting liquid demonstrated high capacity retention (80.1% over 4000 cycles) and Coulombic efficiency (99.7%) when operated at a high current density of 2.2 mA/cm(2) at 25 °C. Furthermore, we successfully demonstrate 100-mAh-level single cells in a pouch cell configuration using a large-area (36 cm(2)) LLZTO solid electrolyte and a 3.2-mAh/cm(2) LiCoO(2) (LCO) positive electrode capable of operating for >400 cycles at a 0.5 C-rate (85 mA/g).