All-solid-state lithium batteries (ASSLBs) are receiving attention as a prospective next-generation secondary battery technology that can reduce the risk of commercial lithium-ion batteries by replacing flammable organic liquid electrolytes with non-flammable solid electrolytes. The practical application of ASSLBs requires developing robust solid electrolytes that possess ionic conductivity at room temperature on a par with that of organic liquids. These solid electrolytes must also be thermally and chemically stable, as well as compatible with electrode materials. Inorganic solid electrolytes, including oxide and sulfide-based compounds, are being studied as promising future candidates for ASSLBs due to their higher ionic conductivity and thermal stability than polymer electrolytes. Here, we present the challenges currently facing the development of oxide and sulfide-based solid electrolytes, as well as the research efforts underway aiming to resolve these challenges.

Li1.5Al0.5Ti1.5(PO4)3 (LATP) is considered to be one of the promising solid-state electrolytes owing to its excellent chemical and thermal stability, wide potential range (~5.0 V), and high ionic conductivity (~10-4 S/cm). LATP powders are typically prepared via the sol-gel method by adding and mixing nitrate or alkoxide precursors with chelating agents. Here, the thermal properties, crystallinity, density, particle size, and distribution of LATP powders based on chelating agents (citric acid, acetylacetone, EDTA) are compared to find the optimal conditions for densely sintered LATP with high purity. In addition, the three types of LATP powders are utilized to prepare sintered solid electrolytes and observe the microstructure changes during the sintering process. The pyrolysis onset temperature and crystallization temperature of the powder samples are in the order AC-LATP > CA-LATP > ED-LATP, and the LATP powder utilizing citric acid exhibits the highest purity, as no secondary phase other than LiTi2PO4 phase is observed. LATP with citric acid and acetylacetone has a value close to the theoretical density (2.8 g/cm3) after sintering. In comparison, LATP with EDTA has a low sintered density (2.2 g/cm3) because of the generation of many pores after sintering.

Supercapacitors are attracting much attention in sensor, military and space applications due to their excellent thermal stability and non-explosion. The ionic liquid is more thermally stable than other electrolytes and can be used as a high temperature electrolyte, but it is not easy to realize a high temperature energy device because the separator shrinks at high temperature. Here, we report a study on electrochemical supercapacitors using a composite electrolyte film that does not require a separator. The composite electrolyte is composed of thermoplastic polyurethane, ionic liquid and fumed silica nanoparticles, and it acts as a separator as well as an electrolyte. The silica nanoparticles at the optimum mass concentration of 4wt% increase the ionic conductivity of the composite electrolyte and shows a low interfacial resistance. The 5 wt% polyurethane in the composite electrolyte exhibits excellent electrochemical properties. At 175 ℃, the capacitance of the supercapacitor using our free standing composite electrolyte is 220 F/g, which is 25 times higher than that at room temperature. This study has many potential applications in the electrolyte of next generation energy storage devices.