• Journal of the Korean Ceramic Society
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• v.56 no.2
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• pp.111-129
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• 2019

Recently, all-solid-state batteries (ASSBs) have attracted increasing interest owing to their higher energy density and safety. As the core material of ASSBs, the characteristics of the solid electrolyte largely determine the performance of the battery. Thus far, a variety of inorganic solid electrolytes have been studied, including the NASICON-type, LISICON-type, perovskite-type, garnet-type, glassy solid electrolyte, and so on. The garnet Li₇La₃Zr₂O₁₂ (LLZO) solid electrolyte is one of the most promising candidates because of its excellent comprehensively electrochemical performance. Both, experiments and theoretical calculations, show that cubic LLZO has high room-temperature ionic conductivity and good chemical stability while contacting with the lithium anode and most of the cathode materials. In this paper, the crystal structure, Li-ion transport mechanism, preparation method, and element doping of LLZO are introduced in detail based on the research progress in recent years. Then, the development prospects and challenges of LLZO as applied to ASSBs are discussed.

• Analytical Science and Technology
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• v.9 no.4
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• pp.382-391
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• 1996

In this study, 12 different chemical species of fine ceramic($BaTiO_3$) were synthesized as the standard materials for the fast and accurate measurements of X-ray fluorescence spectrometry. Samples were diluted to sixteen times with the filling compound ($Li_2B_4O_7+LiBO_2$) in order to remove the matrix effect, and to get the convenient storage and homogeneity of ingredients. The matrix effects among the ingredients were corrected by the empirical coefficient method based on the Lucas-Tooth and Price model. The standard curve on 12 standard materials containing 15 elements were obtained by using X-ray fluorescence spectrometry at three different laboratories. The correlation factors of BaO, PbO, SrO, $Fe_2O_3$, $La_2O_3$, $SnO_2$, ZnO, $ZrO_2$, CaO indicated the relati vely good agreement over 0.995 among the three different laboratories. $SiO_2$ and $Al_2O_3$ showed the poor linearity because of their low fluorescence intensities.

• Journal of Electrochemical Science and Technology
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• v.13 no.2
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• pp.199-207
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• 2022

Lithium-sulfur batteries (LSBs) have emerged as a promising alternative to lithium-ion batteries (LIBs) owing to their high energy density and economic viability. In addition, all-solid-state LSBs, which use solid-state electrolytes, have been proposed to overcome the polysulfide shuttle effect while improving safety. However, the high interfacial resistance and poor ionic conductivity exhibited by the electrode and solid-state electrolytes, respectively, are significant challenges in the development of these LSBs. Herein, we apply a poly (ethylene oxide) (PEO)-based composite solid-state electrolyte with oxide Li₇La₃Zr₂O₁₂ (LLZO) solid-state electrolyte in an all-solid-state LSB to overcome these challenges. We use an electrochemical method to evaluate the degradation of the all-solid-state LSB in accordance with the carbon content and loading weight within the cathode. The all-solid-state LSB, with sulfur-carbon content in a ratio of 3:3, exhibited a high initial discharge capacity (1386 mAh g^-1), poor C-rate performance, and capacity retention of less than 50%. The all-solid-state LSB with a high loading weight exhibited a poor overall electrochemical performance. The factors influencing the electrochemical performance degradation were revealed through systematic analysis.

• Journal of the Korean Electrochemical Society
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• v.21 no.4
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• pp.80-87
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• 2018

Safety issues in Li-ion battery system have been prime concerns, as demands for power supply device applicable to wearable device, electrical vehicles and energy storage system have increased. To solve safety problems, promising strategy is to replace organic liquid electrolyte with non-flammable solid electrolyte, leading to the development of all-solid-state battery. However, relative low conductivity and high resistance from rigid solid-solid interface hinder a wide application of solid electrolyte. Composite electrolytes composed of organic and inorganic parts could be alternative solution, which in turn bring about the increase of conductivity and conformal contact at physically rough interfaces. In our study, composite electrolytes were prepared by combining poly(ethylene oxide)(PEO) and $Li_7La_3Zr_2O_{12}$ (LLZO). The crystallinity, morphology and electrochemical performances were investigated with the control of LLZO contents from 0 wt% to 50 wt%. From the results, it is concluded that optimum content and uniform dispersion of LLZO in polymer matrix are significant to improve overall conductivity of composite electrolyte.

• Journal of the Korean Electrochemical Society
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• v.25 no.3
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• pp.105-112
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• 2022

For the commercialization of all-solid-state batteries, it is essential to develop a solid electrolyte that can be operable at room temperature, and it is necessary to manufacture all-solid-state batteries by adopting materials with high ionic conductivity. Therefore, in order to increase the ionic conductivity of the existing oxide-based solid, Li₇La₃Zr₂O₁₂ (LLZO) doped with heterogeneous elements was used as a filler material (Al and Nb-LLZO). An electrolyte with garnet-type inorganic filler doped was prepared. The binary metal element and the polymer mixture of poly(ethylene oxide)/poly(propylene carbonate) (PEO/PPC) (1:1) are uniformly manufactured at a ratio of 1:2.4, The electrochemical performance was tested at room temperature and 60 ℃ to verify room temperature operability of the all-solid-state battery. The prepared composite electrolyte shows improved ionic conductivity derived from co-doping of the binary elements, and the PPC helps to improve the ionic conductivity, thereby increasing the capacity of all-solid-state batteries at room temperature as well as 60 ℃. It was confirmed that the capacity retention rate was improved.

• Journal of Electrochemical Science and Technology
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• v.14 no.1
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• pp.85-95
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• 2023

In recent years, solid-state Li metal batteries (SSLBs) have attracted significant attention as the next-generation batteries with high energy and power densities. However, uncontrolled dendrite growth and the resulting pulverization of Li during repeated plating/stripping processes must be addressed for practical applications. Herein, we report a plastic-crystal-based polymer/ceramic composite solid electrolyte (PCCE) to resolve these issues. To fabricate the one-side ceramic-incorporated PCCE (CI-PCCE) film, a mixed precursor solution comprising plastic-crystal-based polymer (succinonitrile, SN) with garnet-structured ceramic (Li₇La₃Zr₂O₁₂, LLZO) particles was infused into a thin cellulose membrane, which was used as a mechanical framework, and subsequently solidified by using UV-irradiation. The CI-PCCE exhibited good flexibility and a high room-temperature ionic conductivity of over 10^-3 S cm^-1. The Li symmetric cell assembled with CI-PCCE provided enhanced durability against Li dendrite penetration through the solid electrolyte (SE) layer than those with LLZO-free PCCEs and exhibited long-term cycling stability (over 200 h) for Li plating/stripping. The enhanced Li⁺ transference number and lower interfacial resistance of CI-PCCE indicate that the ceramic-polymer composite layer in contact with the Li anode enabled the uniform distribution of Li⁺ flux at the interface between the Li metal and CI-PCCE, thereby promoting uniform Li plating/stripping. Consequently, the Li//LiFePO₄ (LFP) full cell constructed with CI-PCCE demonstrated superior rate capability (~120 mAh g^-1 at 2 C) and stable cycle performance (80% after 100 cycles) than those with ceramic-free PCCE.