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Critical Review
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A Review of Inorganic Solid Electrolytes for All-Solid-State Lithium Batteries: Challenges and Progress
Seul Ki Choi, Jaehun Han, Gi Jeong Kim, Yeon Hee Kim, Jaewon Choi, MinHo Yang
J Powder Mater. 2024;31(4):293-301.   Published online August 30, 2024
DOI: https://doi.org/10.4150/jpm.2024.00206
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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.
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Effect of Chelating Agent on Li1.5Al0.5Ti1.5(PO4)3 Particles by Sol-gel Method and Densification
SungJoon Ryu, Seul Ki Choi, Jong Ho Won, MinHo Yang
J Powder Mater. 2023;30(5):394-401.   Published online October 1, 2023
DOI: https://doi.org/10.4150/KPMI.2023.30.5.394
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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.

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A Study on the Microstructures and Ionic Conductivity of Li1.3Al0.3Ti1.7(PO4)3 with Different Synthesis Routes
Seul Ki Choi, Jeawon Choi, MinHo Yang
J Powder Mater. 2023;30(2):107-115.   Published online April 1, 2023
DOI: https://doi.org/10.4150/KPMI.2023.30.2.107
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Li1.3Al0.3Ti1.7(PO4)3(LATP) is considered a promising material for all-solid-state lithium batteries owing to its high moisture stability, wide potential window (~6 V), and relatively high ion conductivity (10-3–10-4 S/cm). Solid electrolytes based on LATP are manufactured via sintering, using LATP powder as the starting material. The properties of the starting materials depend on the synthesis conditions, which affect the microstructure and ionic conductivity of the solid electrolytes. In this study, we synthesize the LATP powder using sol-gel and co-precipitation methods and characterize the physical properties of powder, such as size, shape, and crystallinity. In addition, we have prepared a disc-shaped LATP solid electrolyte using LATP powder as the starting material. In addition, X-ray diffraction, scanning electron microscopy, and electrochemical impedance spectroscopic measurements are conducted to analyze the grain size, microstructures, and ion conduction properties. These results indicate that the synthesis conditions of the powder are a crucial factor in creating microstructures and affecting the conduction properties of lithium ions in solid electrolytes.


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