• Journal of the Korean Electrochemical Society
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• v.24 no.4
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• pp.100-105
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• 2021

Recently, all-solid-state batteries have attracted much attention to improve safety of rechargeable lithium batteries, but the solid-state batteries of conductive ceramics or solid polymer electrolytes show poor electrochemical properties because of several problems such as high interfacial resistance and undesired reactions. To solve the problems of the reported all-solid-state batteries, a hybrid solid electrolyte is suggested, in this study, NASICON-type nanoparticle Li_1.5Al_0.5Ti_1.5P₃O₁₂ (LATP) conductive ceramic, PVdF-HFP, and a carbonate-based liquid electrolyte were composited to prepare a quasi-solid electrolyte. The hybrid solid electrolyte has a high voltage stability of 5.6 V and shows an suppress effect of lithium dendrite growth in the stripping-plating test. The LiNi_0.83Co_0.11Mn_0.06O₂ (NCM811)-based battery with the hybrid solid electrolyte exhibits a high discharge capacity of 241.5 mAh/g at a high charge-cut-off voltage of 4.8V and stable electrochemical reaction. The NCM811-based battery also shows 139.4 mAh/g discharge capacity without short circuit or explosion at 90℃. Therefore, the LATP-based hybrid solid electrolyte can be an effective solution to improve the safety and electrochemical properties of rechargeable lithium batteries.

• Corrosion Science and Technology
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• v.23 no.4
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• pp.334-342
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• 2024

The need for efficient and sustainable energy storage solutions has emerged due to a rapidly increasing energy demand and growing concerns about environmental issues. Among various energy storage methods, lithium secondary batteries are widely used in a variety of electronic devices such as smartphones, laptops, electric vehicles, and large-scale power storage systems due to their high energy density, long lifespan, and cost competitiveness. Recently, all-solid-state batteries (ASSBs) have attracted great attention because they can reduce the risk of fire associated with liquid electrolytes. Additionally, using high-capacity alternative anodes and cathodes in ASSBs can enhance energy density. However, ASSBs that use solid electrolytes experience a degradation in their electrochemical performances due to resistance at solid-solid interfaces. These interfaces can also result in poor physical contact and the presence of products formed from chemical and electrochemical reactions. Solving this interface problem is a critical issue for the commercialization of ASSBs. This review summarizes interfacial reactions between the cathode and solid electrolyte, along with research aimed at improving these interactions. Future development directions in this field are also discussed.

• Journal of the Korean Institute of Electrical and Electronic Material Engineers
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• v.36 no.6
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• pp.627-632
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• 2023

Lithium-ion batteries are widely used in various applications, including electric vehicles and portable electronics, due to their high energy density and long cycle life. The performance of lithium-ion batteries can be improved by using solid electrolytes, in terms of higher safety, stability, and energy density. Li_1.5Al_0.5Ti_1.5(PO₄)₃ (LATP) is a promising solid electrolyte for all-solid-state lithium batteries due to its high ionic conductivity and excellent stability. However, the ionic conductivity of LATP needs to be improved for commercializing all-solid-state lithium battery systems. In this study, we investigate the microstructures and ionic conductivities of LATP by incorporating B₂O₃ glass ceramics. The smaller grain size and narrow size distribution were obtained after the introduction of B₂O₃ in LATP, which is attributed to the B₂O₃ glass on grain boundaries of LATP. Moreover, higher ionic conductivity can be obtained after B₂O₃ incorporation, where the optimal composition is 0.1 wt% B₂O₃ incorporated LATP and the ionic conductivity reaches 8.8×10^-5 S/cm, more than 3 times higher value than pristine LATP. More research could be followed for having higher ionic conductivity and density by optimizing the processing conditions. This facile approach for establishing higher ionic conductivity in LATP solid electrolytes could accelerate the commercialization of all-solid-state lithium batteries.

• Proceedings of the Materials Research Society of Korea Conference
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• 1998.08a
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• pp.151.1-151
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• 1998

• Proceedings of the Korean Institute of Electrical and Electronic Material Engineers Conference
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• 1999.11a
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• pp.159-162
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• 1999

All solid state thin film micro-batteries consisting of lithium metal anode, an amorphous LiPON electrolyte and cathode of vanadium oxide have been fabricated and characterized, which were fabricated with cell structure of Li/LiPON/V$_2$O$\sub$5/Pt. The vanadium oxide thin films were formed by d.c. reactive sputtering on Pt current collector. After deposition of vanadium oxide films, in-situ growths of lithium phosphorus oxynitride film were conducted by r.f. sputtering of Li$_3$PO$_4$ target in mixture gas of N$_2$ and O$_2$. The pure metal lithium film was deposited by thermal evaporation on thin film LiPON electrolyte. The cell capacity was about 45${\mu}$Ah/$\textrm{cm}^2$ $\mu\textrm{m}$ after 200 cycle. No appreciable degradation of the cell capacity could be observed after 50 cycles .

• 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 the Korean institute of surface engineering
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• v.51 no.4
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• pp.243-248
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• 2018

All solid state thin film batteries with two types of cell structure, Pt / $LiCoO_2$ / LiPON / Cu and Pt / $LiCoO_2$ / LiPON / $LiCoO_2$ / Cu, are prepared and their electrochemical performances are investigated to evaluate the effect of $LiCoO_2$ interlayer at the interface of LiPON / Cu. The crystallinity of the deposited $LiCoO_2$ thin films is confirmed by XRD and Raman analysis. The crystalline $LiCoO_2$ cathode thin film is obtained and $LiCoO_2$ as the interlayer appears to be amorphous. The surface morphology of Cu current collector after cycling of the batteries is observed by AFM. The presence of a 10 nm-thick layer of $LiCoO_2$ at the interface of LiPON / Cu enhances the interfacial adhesion and reduces the interfacial resistance. As a result, Li plating / stripping at the interface of LiPON / Cu during charge/discharge reaction takes place more uniformly on Cu current collector, while without the interlayer of $LiCoO_2$ at the interface of LiPON / Cu, the Li plating / stripping is localized on current collector. The thin film batteries with the interlayer of $LiCoO_2$ at the interface of LiPON / Cu exhibits enhanced initial coulombic efficiency, reversible capacity and cycling stability. The thickness of the anode current collector Cu also appears to be crucial for electrochemical performances of all solid state thin film batteries.

• Applied Chemistry for Engineering
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• v.33 no.1
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• pp.58-63
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• 2022

Graphite has been used as an anode material for lithium-ion batteries for the past 30 years due to its low de-/lithiation voltage, high theoretical capacity of 372 mAh/g, low price, and long life properties. Recently, all-solid-state lithium-ion batteries (ASSLB), which are composed of inorganic solid materials with high stability, have received great attention as electric vehicles and next-generation energy storage devices, but research works on graphite that works well for ASSLB systems are insufficient. Therefore, we induced the performance improvement of ASSLB anode electrode graphite material by removing the amorphous carbon present in the carbon material surface, acting as a resistive layer from the graphite. As a result of X-ray diffraction (XRD) analysis using heat treated graphite in air at 400, 500, and 600 ℃, the full width at half maximum (FWHM) at (002) peak was reduced compared to that of bare graphite, indicating that the crystallinity of graphite was improved after heat treatment. In addition, the discharge capacity, initial coulombic efficiency (ICE) and cycle stability increased as the crystallinity of graphite increased after heat treatment. In the case of graphite annealed in air at 500 ℃, the high capacity retention rate of 331.1 mAh/g and ICE of 86.2% and capacity retention of 92.7% after 10-cycle measurement were shown.

• Journal of the Korean Institute of Electrical and Electronic Material Engineers
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• v.37 no.4
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• pp.445-450
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• 2024

The expansion of lithium-ion battery usage beyond portable electronic devices to electric vehicles and energy storage systems is driven by their high energy density and favorable cycle characteristics. Enhancing the stability and performance of these batteries involves exploring solid electrolytes as alternatives to liquid ones. While sulfide-based solid electrolytes have received significant attention for commercialization, research on amorphous-phase glass solid electrolytes in oxide-based systems remains limited. Here, we investigate the glass transition temperatures and sintering behaviors by changing the molecular ratio of Li₂O/B₂O₃ in borate glass comprising Li₂O-B₂O₃-Al₂O₃ system. The glass transition temperature is decreasing as increasing the amount of Li₂O. When we sintered at 450℃, just above the glass transition temperature, the samples did not consolidate well, while the proper sintered samples could be obtained under the higher temperature. We successfully obtained the borate glass ceramics phases by melt-quenching method, and the sintering characteristics are investigated. Future studies could explore optimizing ion conductivity through refining processing conditions, adjusting the glass former-to-modifier ratio, and incorporating additional Li salt to enhance the ionic conductivity.

• Journal of the Korean Electrochemical Society
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• v.25 no.3
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• pp.95-104
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• 2022

The development of non-flammable all-solid-state batteries (ASSLBs) has become a hot topic due to the known drawbacks of commercial lithium-ion batteries. As the possibility of applying sulfide solid electrolytes (SSEs) for electric vehicle batteries increases, efforts for the low-cost mass-production are actively underway. Until now, most studies have used high-energy mechanical milling, which is easy to control composition and impurities and can reduce the process time. Through this, various SSEs that exceed the Li⁺ conductivity of liquid electrolytes have been reported, and expectations for the realization of ASSLBs are growing. However, the high-energy mechanical milling method has disadvantages in obtaining the same physical properties when mass-produced, and in controlling the particle size or shape, so that physical properties deteriorate during the full process. On the other hand, wet chemical synthesis technology, which has advantages in mass production and low price, is still in the initial exploration stage. In this technology, SSEs are mainly manufactured through producing a particle-type, solution-type, or mixed-type precursor, but a clear understanding of the reaction mechanism hasn't been made yet. In this review, wet chemical synthesis technologies for SSEs are summarized regarding the reaction mechanism between the raw materials in the solvent.