Abstract
Garnet-type solid electrolytes have attracted extensive attention for solid-state lithium (Li) batteries. However, the high processing temperature of up to 1,200°C limits large-scale production. Here, we report a simple approach to reduce the sintering temperature by using a conformal nanoscale amorphous alumina coating. The ceramic sintered at 980°C shows a high room temperature ionic conductivity of 0.13 mS cm−1. It reveals that the second phases segregated at grain boundaries are ionically conductive but electronically blocking, which can block electronic conduction and improve mechanical property. The Li symmetry cells indicate a long-term 2,500-cycle life and a high critical current density of 0.52 mA cm−2. The garnet electrolyte enables the high-voltage cells using Li1.2Ni0.2Mn0.6O2 to deliver a high specific capacity of 248 mAh g−1 at 0.05 C. This work provides a new clue for lowering sintering temperature for garnet electrolytes, which can extend to other ceramics toward practical applications.
Highlights
Lithium-ion batteries (LIBs) as energy storage devices are widely used in commercial electronics and electric vehicles
Garnet-type oxide electrolyte Li7La3Zr2O12 (LLZO) has attracted increasing attention owing to its high room-temperature (RT) ionic conductivity (10-4-10-3 S cm-1), wide electrochemical potential window, and high chemical stability against Li metal[9,10,11]
The LLZO ceramic exhibits high Young’s modulus (~150 GPa) and shear modulus (~60 GPa)[12,13], which is expected to suppress Li dendrite growth according to Newman and Monroe’s prediction[14]
Summary
Lithium-ion batteries (LIBs) as energy storage devices are widely used in commercial electronics and electric vehicles. The forming Li-Al-O second phase uniformly distributed at the grain boundaries can effectively enhance sintering activity and subsequently promote the densification.
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