• Journal of Electrochemical Science and Technology
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• v.13 no.3
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• pp.362-368
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• 2022

The application of polymer composite electrolyte in all-solid-state lithium-sulfur battery (ASSLSBs) can guarantee high energy density and improve the interface contact between electrolyte and electrode, which has a broader application prospect. However, the inherent insulation of the sulfur-cathode leads to a low electron/ion transfer rate. Carbon materials with high electronic conductivity and electrolyte materials with high ionic conductivity are usually selected to improve the electron/ion conduction of the composite cathode. In this work, PEO-LiTFSI-LLZO composite polymer electrolyte (CPE) with high ionic conductivity was prepared. The ionic conductivity was 1.16×10^-4 and 7.26×10^-4 S cm^-1 at 20 and 60℃, respectively. Meanwhile, the composite sulfur cathode was prepared with Sulfur, reduced graphene oxide and composite polymer electrolyte slurry (S-rGO-CPEs). In addition to improving the ion conductivity in the cathode, CPEs also replaces the role of binder. The influence of different contents of CPEs in the cathode material on the performance of the constructed battery was investigated. The results show that the electrochemical performance of the all-solid-state lithium-sulfur battery is the best when the content of the composite electrolyte in the cathode is 40%. Under the condition of 0.2C and 45℃, the charging and discharging capacity of the first cycle is 923 mAh g^-1, and the retention capacity is 653 mAh g^-1 after 50 cycles.

• Journal of the Korean Institute of Electrical and Electronic Material Engineers
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• v.33 no.5
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• pp.411-417
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• 2020

In this study, we introduce a Na β"-alumina composite thick film as a solid electrolyte, to reduce the resistance of electrolyte for a Na/S battery. An alumina/zirconia composite material was used to enhance the mechanical properties of the electrolyte. A solid electrolyte of about 40 ㎛ thick was successfully fabricated through the conversion and tape-casting methods. In order to investigate the effect of the surface treatment process of the solid electrolyte on the battery performance, the electrolyte was polished by dry and wet processes, respectively, and then the Na/S batteries were prepared for analyzing the battery characteristics. The battery with the dry process performed much better than the battery made with the wet process. As a result, the battery manufactured by the dry process showed excellent performance. Therefore, it is confirmed that the surface treatment process of the solid electrolyte has an important effect on the battery capacity and coulombic efficiency, as well as the interface reaction.

• Journal of the Semiconductor & Display Technology
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• v.21 no.3
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• pp.114-118
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• 2022

The stabilized all-solid-state battery structure indicate a fundamental alternative to the development of next-generation energy storage devices. Existing liquid electrolyte structures severely limit battery stability, creating safety concerns due to the growth of Li dendrites during rapid charge/discharge cycles. In this study, a low-dimensional graphene quantum dot layer structure was applied to demonstrate stable operating characteristics based on Li+ ion conductivity and excellent electrochemical performance. Transmission electron microscopy analysis was performed to elucidate the microstructure at the interface. The low-dimensional structure of GQD-based solid electrolytes has provided an important strategy for stable scalable solid-state lithium battery applications at room temperature. This study indicates that the low-dimensional carbon structure of Li-GQDs can be an effective approach for the stabilization of solid-state Li matrix architectures.

• Journal of the Korean Electrochemical Society
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• v.22 no.3
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• pp.87-103
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• 2019

Nonaqueous organic electrolyte solution in commercially available lithium-ion batteries, due to its flammability, corrosiveness, high volatility, and thermal instability, is demanding to be substituted by safer solid electrolyte with higher cycle stability, which will be utilized effectively in large-scale power sources such as electric vehicles and energy storage system. Of various types of solid electrolytes, composite solid electrolytes with polymer matrix and active inorganic fillers are now most promising in achieving higher ionic conductivity and excellent interface contact. In this review, some kinds and brief history of solid electrolyte are at first introduced and consequent explanations of polymer solid electrolytes and inorganic solid electrolytes (including active and inactive fillers) are comprehensively carried out. Composite solid electrolytes including these polymer and inorganic materials are also described with their electrochemical properties in terms of filler shapes, such as particle (0D), fiber (1D), plane (2D), and solid body (3D). In particular, in all-solid-state lithium batteries using lithium metal anode, the interface characteristics are discussed in terms of cathode-electrolyte interface, anode-electrolyte interface, and interparticle interface. Finally, current requisites and future perspectives for the composite solid electrolytes are suggested by help of some decent reviews recently reported.

• 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.

• 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.

• Korean Journal of Materials Research
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• v.29 no.2
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• pp.121-128
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• 2019

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 $175^{\circ}C$, 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.

• Journal of Ceramic Processing Research
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• v.19 no.5
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• pp.413-418
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• 2018

All-solid-state lithium batteries (ASSBs) using inorganic sulfide-based solid electrolytes are considered prospective alternatives to existing liquid electrolyte-based batteries owing to benefits such as non-flammability. However, it is difficult to form a favorable solid-solid interface among electrode constituents because all the constituents are solid particles. It is important to form an effective electron conduction network in composite cathode while increasing utilization of active materials and not blocking the lithium ion path, resulting in excellent cell performance. In this study, a mixture of fibrous VGCF and spherical nano-sized Super P was used to improve rate performance by fabricating valid conduction paths in composite cathodes. Then, composite cathodes of ASSBs containing 70% and 80% active materials ($LiNi_{0.6}Co_{0.2}Mn_{0.2}O_2$) were prepared by a solution-based process to achieve uniform dispersion of the electrode components in the slurry. We investigated the influence of binary carbon additives in the cathode of all-solid-state batteries to improve rate performance by constructing an effective electron conduction network.

• Journal of the Korean Ceramic Society
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• v.48 no.1
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• pp.110-115
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• 2011

$Gd_2O_3$-doped $CeO_2$ (GDC) and $La_{0.6}Sr_{0.4}Co_{0.2}Fe_{0.8}O_3$ (LSCF) composite cathode materials were prepared in order to be applied to intermediate-temperature solid oxide fuel cells. The electrochemical polarization was evaluated using ac impedance spectroscopy involving geometric restriction at the interface between an ionic electrolyte and a mixed-conducting cathode. In order to optimize the cathode composites applicable to a GDC electrolyte, the cathode composites were evaluated in terms of polarization losses with regard to a given electrolyte, i.e., GDC electrolyte. The polarization increased significantly with decreasing temperature and was critically dependent on the compositions of the composite cathodes. The optimized cathode composite was found to consist of GDC 50 wt% and LSCF 50 wt%; the corresponding normalized polarization loss was calculated to be 0.64 at $650^{\circ}C$.

• Journal of the Korean Electrochemical Society
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• v.19 no.3
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• pp.101-106
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• 2016

In this study, we prepared an ionic liquid composite solid polymer electrolyte (PEO-LiTFSI-$Pyr_{14}TFSI$) with poly(ethylen oxide), lithium bis(trifluoromethanesulfonyl)imide, N-butyl-N-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide by blending-cross linking process. Although the PEO-LiTFSI-$Pyr_{14}TFSI$ composite solid polymer electrolyte displayed a small peak at 4.4 V, it had high electrochemical oxidation stability up to 5.7 V. Ionic conductivity of the PEO-LiTFSI-$Pyr_{14}TFSI$ composite solid polymer electrolyte increased with increasing temperature from $10^{-6}S\;cm^{-1}$ at $30^{\circ}C$ to $10^{-4}S\;cm^{-1}$ at $70^{\circ}C$. To investigate the electrochemical properties, the PEO-LiTFSI-$Pyr_{14}TFSI$ composite solid polymer electrolyte assembled with $LiFePO_4$ cathode and Li-metal anode. At 0.1 C-rate, the cell delivered $40mAh\;g^{-1}$ for $30^{\circ}C$, $69.8mAh\;g^{-1}$ for $40^{\circ}C$ and $113mAh\;g^{-1}$ for $50^{\circ}C$, respectively. The PEO-LiTFSI-$Pyr_{14}TFSI$ solid polymer electrolyte exhibited good charge-discharge performance in Li/SPE/$LiFePO_4$ cells at $50^{\circ}C$.