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As one of the most promising next-generation energy storage device, lithiummetal batteries have been extensively investigated. However, the poor safetyissue and undesired lithium dendrites growth hinder the development of lithiummetal batteries. The application of solid state electrolytes has attractedincreasing attention as they can solve the safety issue and partly inhibit thegrowth of lithium dendrites. Polyethylene oxide (PEO)-based electrolytes arevery promising due to their enhanced safety and excellent flexibility. However,PEO-based electrolytes suffer from low ionic conductivity at room temperatureand can't effectively inhibit lithium dendrites at high temperature due to theintrinsic semi-crystalline properties and poor mechanical strength. In thiswork, a novel coral-like Li6.25Al0.25La3Zr2O12 (LALZO) is synthesized to use asan active ceramic filler in PEO. The PEO with LALZO coral (PLC) exhibitsincreased ionic conductivity and mechanical strength, which leads to theuniform deposition/stripping of lithium metal. The Li symmetric cells with PLCcycle for 1500 h without short circuit at 50 centidegree. The assembledLiFePO4/PLC/Li batteries display excellent cycling stability at both 60 and 50centidegree. This work reveals that the electrochemical properties of organicand inorganic composite electrolyte can be effectively improved by tuning themicrostructure of the filler, such as the coral-like LALZO architecture.

Synergistic Effect of One- and Two-dimensional Connected Coral-like  Li$_{6.25}$Al$_{0.25}$La$_3$Zr$_2$O$_{12}$ in PEO-Based Composite Solid State  Electrolyte