PUBLICATION
Advanced Materials for Energy Storage Lab.
PUBLICATION
Advanced Materials for Energy Storage Lab.
Garnet-type Li7La3Zr2O12 (LLZO) is a promising electrolyte for solid-state lithium metal batteries owing to its high ionic conductivity and chemical stability towards lithium metal. High-temperature sintering (over 1100 °C) is essential for the fabrication and production of LLZO, which is often challenged by elemental loss (i.e. lithium volatilization) during sintering and thus causes product reliability issues. Here, we propose a simple and scalable coating strategy to enable LLZO to be sintered efficiently without sacrificial mother powder. We reveal that multifunctional Li-Al-O compounds coated on LLZO electrolytes effectively promote sintering process while mitigating lithium loss upon conventional high-temperature sintering, rendering a highly dense (98.2%) sintered pellet with high ionic conductivity (8.82 × 10−4 S cm-1) and low electronic conductivity (7.59 × 10−10 S cm-1). The fabricated pellets exhibit a significantly enhanced critical current density along with low charge-transfer resistance at the interface with lithium metals, attributable to the lithophilic Li-Al-O compound that is uniformly distributed across the particles/grain boundaries. Furthermore, we demonstrate the practical viability of the strategy by showcasing the fabrication of high-quality supersized pellets with arial size up to 16 cm2 (after sintering). We expect that this simple yet effective strategy involving multifunctional agents to simultaneously design materials and their fabrication process expedites the technological advancement of sintering for solid-state oxide electrolytes towards commercialization.