Enhanced ionic conductivity of composite solid electrolyte by defective Li1.3Al0.3Ti1.7(PO4-y)3 for solid-state Li-ion batteries

Oxygen-deficient Li1.3Al0.3Ti1.7(PO4)3 (LATP) was prepared using a hydrothermal method followed by high-temperature calcination. Comprehensive analyses using X-ray powder diffraction (XRD), electron paramagnetic resonance (EPR), and X-ray photoelectron spectroscopy (XPS) conclusively demonstrated the successful preparation of oxygen-deficient LATPs under different calcination temperatures in an argon-hydrogen mixed atmosphere. These varying temperatures affected the concentration of oxygen defects in LATP. The hydrothermal precursor was calcined at 700 °C for 6 h to prepare an oxygen-deficient LATP, which was subsequently combined with polyacrylonitrile (PAN) to form a solid composite electrolyte. The composite exhibited a total ionic conductivity of 7.55 × 10−4 S cm−1 at 20 °C. Furthermore, when tested at 25 °C with a current density of 0.025 mA cm−2, the composite displayed good compatibility with a lithium metal anode. At a current density of 0.1 C, the initial discharge capacity was found to be 256.2 mA h g−1, which was maintained at 231.8 mA h g−1 after 100 cycles within the voltage range of 2.0–4.5 V. By judiciously modulating the oxygen defects concentration, it is possible to not only improve the ionic conductivity of the solid composite electrolyte but also to further enhance its discharge capacity.