Abstract
Novel LLZTO@Li4GeO4/Li2O composite electrolytes have been successfully produced through liquid sintering Li6.4La3Zr1.4Ta0.6O12 via the 3Li2O-2GeO2 (LGO1.5) additive at 1140 °C for 3 h in air atmosphere. The Li-Ge-O additive performs a prominent role in fabricating compact connections among LLZTO grains and accelerating their densification procedure. Moreover, the additive acts as a bridge to promote Li+ transportation in the grain boundary domains. Consecutive Li+ conduction pathways are constructed inside the ceramics correspondingly. A considerably enhancement for the electrical performance of the garnet-type electrolytes is realized. The composite electrolyte with 2wt% LGO1.5 exhibits a high ionic conductivity of 5.57 × 10−4 S·cm‒1 at 25 °C, the relative density of which reaches 95.8%. It is also capable of withstanding a high voltage up to 6 V (vs. Li/Li+) and a large critical current density of 0.65 mA·cm‒2.
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