• Ceramist
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• v.22 no.2
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• pp.170-181
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• 2019

All-solid-state batteries have received increasing attention because of their high safety aspect and high energy and power densities. However, the inferior solid-solid interfaces between solid electrolyte and active materials in electrode, which cause high interfacial resistance, reduce ion and electron transfer rate and limit battery performance. Recently, spark plasma sintering is emerging as a promising technique for fabricating solid electrolytes and composite-electrodes. Herein, this paper focuses on the overview of spark plasma sintering to fabricate solid electrolytes and composite-electrodes for all-solid-state batteries. In the end, future opportunities and challenges associated with SPS technique for all-solid-state batteries are described.

• 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 Electrochemical Science and Technology
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• v.9 no.3
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• pp.176-183
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• 2018

In this study, a $Li_2ZrO_3$ coated $Li[Ni_{0.8}Co_{0.15}Al_{0.05}]O_2$ (NCA) cathode was applied to an all-solid-state cell employing a sulfide-based solid electrolyte. Sulfide-based solid electrolytes are preferable for all-solid-state cells because of their high ionic conductivity and good softness and elasticity. However, sulfides are very reactive with oxide cathodes, and this reduces the stability of the cathode/electrolyte interface of all-solid-state cells. $Li_2ZrO_3$ is expected to be a suitable coating material for the cathode because it can suppress the undesirable reactions at the cathode/sulfide electrolyte interface because of its good stability and high ionic conductivity. Cells employing $Li_2ZrO_3$ coated NCA showed superior capacity to those employing pristine NCA. Analysis by X-ray photoelectron spectroscopy and electron energy loss spectroscopy confirmed that the $Li_2ZrO_3$ coating layer suppresses the propagation of S and P into the cathode and the reaction between the cathode and the sulfide solid electrolyte. These results show that $Li_2ZrO_3$ coating is promising for reducing undesirable side reactions at the cathode/electrolyte interface of all-solid-state-cells.

• Journal of Industrial Technology
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• v.42 no.1
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• pp.19-27
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• 2022

This review will discuss the effort to understand the interfacial reactions at the anode and cathode sides of all-solid-state batteries. Antiperovskite solid electrolytes have received increasing attention due to their low melting points and anion tunability which allow controlling microstructure and crystallographic structures of this material system. Antiperovskite solid electrolytes pave the way for the understanding relationship between critical current density and mechanical properties of solid electrolytes. Microstructure engineering of cathode materials has been introduced to mitigate the volume change of cathode materials in solid-state batteries. The hollow microstructure coupled with a robust outer oxide layer effectively mitigates both volume change and stress level of cathode materials induced by lithium insertion and extraction, thus improving the structural stability of the cathode and outer oxide layer, which results in stable cycling performance of all-solid-state batteries.

• Journal of the Korean Chemical Society
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• v.67 no.3
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• pp.165-174
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• 2023

The development of all-solid-state batteries (ASSBs) has been gaining attention in recent years due to their potential to offer higher energy densities, improved safety, and longer cycle life compared to conventional lithium-ion batteries. However, several challenges must be addressed to achieve the practical application of ASSBs, such as the development of high-performance solid-state electrolytes, stable electrode-electrolyte interfaces, and cost-effective manufacturing processes. In this review paper, we present an overview of the current state of ASSB research, including recent progress in solid-state electrolyte and cathode/anode materials, and cell architecture. We also summarize the recent advancements and highlight the remaining challenges in ASSB research, with an outlook on the future of this promising technology.

• 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 Institute of Electrical and Electronic Material Engineers
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• v.17 no.9
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• pp.930-935
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• 2004

$({Li}_{0.5}0{La}_{0.5}){TiO}_3$ (LLTO) solid electrolyte was grown on LiCo{O}_2 (LCO) cathode films deposited on $Pt/Ti{O}-2/Si{O}_2/Si$ substrate using pulsed laser deposition for all-solid-state lithium microbattery. LLTO solid electrolyte exhibits an amorphous phase at various deposition temperatures. LLTO films deposited at 10$0^{\circ}C$ showed a clear interrace without any chemical reaction with LCO, and showed an initial discharge capacity of 50 $\mu$Ah/cm$^2$-$\mu$m and capacity retention of 90 % after 100 cycles with Li anode in 1mol$ LiCl{O}_4$ in propylene carbonate (PC). The increase of capacity retention in LLTO/LCO structure than LCO itself was attributed to the structural stability of LCO cathode films by the stacked LLTO. The cells of LLTO/LCO with LLTO grown at $100^{\circ}C$ showed a good cyclic property of 63.6 % after 300 cycles. An amorphous LLTO solid electrolyte is possible for application to solid electrolyte for all-solid-state lithium microbattery.

• Proceedings of the Korean Institute of Electrical and Electronic Material Engineers Conference
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• 1996.05a
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• pp.295-298
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• 1996

In this study, we have fabricated all solid state electrochromic devices using WO$_3$ film as the working electrode, V$_2$O$\_$5/ film as the counter electrode and PEO-LiClO$_4$-PC film as the solid electrolyte. The WO$_3$ thin films for working electrode and V$_2$O$\_$5/ thin films for counter electrode were deposited onto ITO glass by vacuum evaporation and were shown good electrochromic and state properties after 1x10$\^$5/ cycles. PEO-LiClO$_4$-PC polymer electrolyte can easily be formed into thin films, do not absorb in the visible region of the light. Therefore, such electrolyte have electrochromic properties suitable for large-scale all solid-state electrochromic devices. All solid-staeelectrochromic devices fabricated in this polymer electrolyte have optical modulation of 20%∼30% at 1.5 V.

• 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.4
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• pp.139-147
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• 2019

Lithium-ion battery (LiB) with high energy density and efficiency has been utilized for the electric vehicle (EV) and energy storage system (ESS) as well as portable devices. However, as explosion accidents have frequently happened till lately, all-solid-state lithium secondary battery (ALSB) began to get in a spotlight because it can secure a very high safety and energy density by substituting flammable organic liquid electrolyte to nonflammable inorganic solid electrolyte. In spite of ALSB's certain merits, it has shown much poorer performance of cells than one of LiB due to some challenges, which have been small or never dealt with in the LiB system. Hence, although plenty of studies made progress to solve them, an approach about design of all-solid-state electrode (ASSE) has been limited on account of difficulty of ALSB's experiments. That is why the virtual 3D structure of an all-solid-state electrode has to be built and used for the prediction of cell performance. In this study, we elucidate how to form the 3D ASSE structure and what to be needed for the simulation of characteristics on ALSB. Furthermore, the ultimate orientation of 3D modeling and simulation for the study of ALSB are briefly suggested.