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Ceramic–polymer composite electrolytes (CPEs) are being explored to achieve both high ionic conductivity and mechanical flexibility. Here, we show that, by incorporating 10 wt % (3 vol %) mixed-sized fillers of Li7La3Zr2O12 (LLZO) doped with Nb/Al, the room-temperature ionic conductivity of a polyvinylidene fluoride (PVDF)–LiClO4-based composite can be as high as 2.6 × 10–4 S/cm, which is 1 order of magnitude higher than that with nano- or micrometer-sized LLZO particles as fillers. The CPE also shows a high lithium-ion transference number of 0.682, a stable and low Li/CPE interfacial resistance, and good mechanical properties favorable for all-solid-state lithium-ion battery applications. X-ray photoelectron spectroscopy and Raman analysis demonstrate that the LLZO fillers of all sizes interact with PVDF and LiClO4. High packing density (i.e., lower porosity) and long conducting pathways are believed responsible for the excellent performance of the composite electrolyte filled with mixed-sized ionically conducting ceramic particles.

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Garnet-type cubic LiLaZrO exhibits one of the highest lithium-ion conductivity values amongst oxides (up to ∼2 mS cm at room temperature). This compound has also emerged as a promising candidate for solid electrolytes in all-solid-state lithium batteries, due to its high ionic conductivity, good chemical stability against lithium metal, and wide electrochemical stability window. Defect chemistry of this class of materials, although less studied, is critical to the understanding of the nature of ionic conductivity and predicting the properties of grain boundaries and heterogeneous solid interfaces. In this study, the electrical properties of nominally undoped cubic LiLaZrO are characterized as a function of temperature and pO using a suite of AC impedance and DC polarization techniques. The formation of ionic defects and defect pairs as well as their impact on the transport properties are discussed, and a Brouwer-type diagram is constructed.

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