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Three-dimensional Garnet Framework Reinforced Solid Composite Electrolytes with High Lithium-Ion Conductivity and Excellent Stability.

We report a three-dimensional garnet framework reinforced solid composite electrolyte with enhanced Li-ion conductivity and thermal, mechanical and electrochemical stability. The 3D garnet framework is fabricated via the polymeric sponge method, using the low-cost polyurethane foam as template. The interconnected 3D garnet framework not only reinforces the composite electrolyte, but also forms continuous Li-ion transport pathways, therefore, increasing the ionic conductivity. The 3D garnet composite electrolyte shows an ionic conductivity of 1.2×10-4 S cm-1 at 30 °C, about two times as high as that of the garnet particle reinforced composite electrolyte. The Li-Li symmetric cell based on the 3D garnet composite electrolyte can be cycled more than 360 h without short-circuit, suggesting an excellent ability to suppress Li-dendrites. The LiFePO4/3D garnet composite electrolyte/Li battery demonstrates excellent cycling performance at 0.5 C. Owing to the cost-saving characteristics, the 3D garnet reinforced solid composite electrolyte is promising for mass production.