Synthesis of Quasi-Solid Electrolytes from High-Strength and Highly Oriented LLZO Porous Ceramics

Quasi-solid-state electrolytes (QSSEs) exhibit improved interfacial interactions and heightened resistance to lithium dendrite penetration. While directed ion transport can considerably reduce the ion-transport distance, fabricating highly oriented garnet-based ceramic frameworks of appropriate strength presents a challenge. Overcoming this hurdle, highly oriented porous garnet ceramics of exceptional mechanical strength have been developed via hot pressing for the first time, yielding QSSEs with high ionic conductivity (4.2 × 10–3 S cm–1) and favorable compatibility with lithium anodes. The LiFePO4/Li full cells assembled with these QSSEs demonstrated a discharge capacity of 145.6 mAh g–1 at 2 C, maintaining a Coulombic efficiency above 99% after 800 cycles with a capacity retention rate of 90.3%. This interconnected garnet framework design offers a novel direction for the development of highly oriented QSSEs.