• 한국재료학회지
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• 제31권11호
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• pp.614-618
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• 2021

As the size of market for electric vehicles and energy storage systems grows, the demand for lithium-ion batteries (LIBs) is increasing. Currently, commercial LIBs are fabricated with liquid electrolytes, which have some safety issues such as low chemical stability, which can cause ignition of fire. As a substitute for liquid electrolytes, solid electrolytes are now being extensively studied. However, solid electrolytes have disadvantages of low ionic conductivity and high resistance at interface between electrode and electrolyte. In this study, Li₇La₃Zr₂O₁₂ (LLZO), one of the best ion conducting materials among oxide based solid electrolytes, is fabricated through RF-sputtering and various electrochemical properties are analyzed. Moreover, the electrochemical properties of LLZO are found to significantly improve with co-sputtered Li₂O. An all-solid thin film battery is fabricated by introducing a thin film solid electrolyte and an Li₄Ti₅O₁₂ (LTO) cathode; resulting electrochemical properties are also analyzed. The LLZO/Li₂O (60W) sample shows a very good performance in ionic conductivity of 7.3×10^-8 S/cm, with improvement in c-rate and stable cycle performance.

• 전기화학회지
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• 제25권3호
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• pp.95-104
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• 2022

상용 리튬이온전지의 에너지밀도 한계와 안전성 이슈로 불연성 전고체전지 개발이 현안이 되고 있다. 특히, 전기자동차를 위한 차세대 이차전지에 황화물 고체전해질의 적용 가능성이 높아지면서, 고체전해질의 대량생산과 저가격화를 위한 노력 또한 활발해 진행되고 있다. 황화물 고체전해질에 관한 현재까지의 대부분의 연구에서는 조성 및 불순물 제어가 용이하고 균질화와 열처리 시간을 줄일 수 있는 고에너지 기계적 밀링법을 이용하여 열역학적으로 안정한 상 및 준-안정한 상에 대한 탐색을 수행해 왔다. 이를 통해 액체 전해질의 리튬이온전도도를 능가하는 다양한 황화물 고체전해질이 보고되어, 고에너지밀도 고안전성 전고체전지 구현에 대한 기대가 커지고 있다. 그러나, 고에너지 기계적 밀링법은 대량생산에 따른 동일 물성 획득이 쉽지 않고, 입도나 형상 제어가 용이하지 않으며, 분쇄-분급 과정에서 물성의 열화가 발생하는 단점이 알려져 있다. 이에 비해 대량생산과 저가격화에 유리한 습식 합성기술은 아직 다양한 고체전해질 제조에 응용되지는 못하고 있다. 습식 합성기술에서는 입자형, 용액형, 또는 혼합형으로 전구체를 합성하고 용매를 제거한 후 열처리하는 공정을 통해 제조하고 있으나, 전구체의 형성 메커니즘에 대한 명확한 규명도 아직 이루어지지 않고 있다. 본 총설에서는 용매 내 원료들의 반응 메커니즘을 중심으로 한 황화물 고체전해질의 습식 합성기술 동향을 살펴보고자 한다.

• 에너지공학
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• 제20권2호
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• pp.109-122
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• 2011

온실가스배출억제와 수입원유저감을 위하여 전 전기자동차의 도입이 활발하게 추진되고 있다. 이의 항속거리 연장을 위한 리튬이온 이차전지 소재와 공정개발 등의 연구개발 동향, 그리고 양산체제 구축 중에 있는 리튬이온 이차전지 메이커의 계획도 조사하였다. 완성차메이커와는 수평분업적인 협력관계가 형성되고 있음을 볼 수 있었다.

• Journal of Electrochemical Science and Technology
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• 제11권3호
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• pp.282-290
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• 2020

In this article, we report the effect of blended cathode materials on the performance of all-solid-state lithium-ion batteries (ASLBs) with oxide-based organic/inorganic hybrid electrolytes. LiFePO₄ material is good candidates as cathode material in PEO-based solid electrolytes because of their low operating potential of 3.4 V; however, LiFePO₄ suffers from low electric conductivity and low Li ion diffusion rate across the LiFePO₄/FePO₄ interface. Particularly, monoclinic Li₃V₂(PO₄)₃ (LVP) is a well-known high-power-density cathode material due to its rapid ionic diffusion properties. Therefore, the structure, cycling stability, and rate performance of the blended LiFePO₄/Li₃V₂(PO₄)₃ cathode material in ASLBs with oxidebased inorganic/organic-hybrid electrolytes are investigated by using powder X-ray diffraction analysis, field-emission scanning electron microscopy, Brunauer-Emmett-Teller sorption experiments, electrochemical impedance spectroscopy, and galvanostatic measurements.

• 한국수소및신에너지학회논문집
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• 제33권5호
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• pp.574-582
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• 2022

A lithium-ion battery exhibits high energy density but has many limitations due to safety issues. Currently, as a solution for this, research on solid state batteries is attracting attention and is actively being conducted. Among the solid electrolytes, sulfide-based solid electrolytes are receiving much attention with high ion conductivity, but there is a limit to commercialization due to the relatively high price of lithium sulfide, which is a precursor material. This study focused on the possibility of relatively inexpensive and light lithium hydride and conducted an experiment on it. In order to analyze the characteristics of LiAlH₄, ion conductivity and thermal stability were measured, and a composites mixed with PVDF, a representative polymer electrolyte, was synthesized to confirm a change in characteristics. And metallurgical changes in the material were performed through XRD, SEM, and BET analysis, and ion conductivity and thermal stability were measured by EIS and LFA methods. As a result, Li₃AlH₆ having ion conductivity higher than LiAlH₄ is formed by the synthesis of composite materials, and thus ion conductivity is slightly improved, but thermal stability is rapidly degraded due to structural irregularity.

• 한국표면공학회지
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• 제51권4호
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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.

• Journal of Electrochemical Science and Technology
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• 제13권3호
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• pp.407-415
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• 2022

Surface coating of cathodes is an essential process for all-solid-state batteries (ASSBs) based on sulfide electrolytes as it efficiently suppresses interfacial reactions between oxide cathodes and sulfide electrolytes. Based on computational calculations, Li₃PO₄ has been suggested as a promising coating material because of its higher stability with sulfides and its optimal ionic conductivity. However, it has hardly been applied to the coating of ASSBs due to the absence of a suitable coating process, including the selection of source material that is compatible with ASSBs. In this study, polyphosphoric acid (PPA) and (NH₄)₂HPO₄ were used as source materials for preparing a Li₃PO₄ coating for ASSBs, and the properties of the coating layer and coated cathodes were compared. The Li₃PO₄ layer fabricated using the (NH₄)₂HPO₄ source was rough and inhomogeneous, which is not suitable for the protection of the cathodes. Moreover, the water-based coating solution with the (NH₄)₂HPO₄ source can deteriorate the electrochemical performance of high-Ni cathodes that are vulnerable to water. In contrast, when an alcohol-based solvent was used, the PPA source enabled the formation of a thin and homogeneous coating layer on the cathode surface. As a consequence, the ASSBs containing the Li₃PO₄-coated cathode prepared by the PPA source exhibited significantly enhanced discharge and rate capabilities compared to ASSBs containing a pristine cathode or Li₃PO₄-coated cathode prepared by the (NH₄)₂HPO₄ source.

• 신재생에너지
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• 제20권2호
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• pp.71-81
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• 2024

In this study, the electrochemical properties of garnet-structured all-solid-state battery electrolytes (Li_6.4La₃Zr_1.4Ta_0.6O₁₂, hereafter LLZTO) were assessed by altering the calcination temperature, while maintaining a consistent sintering duration. Among the various heat treatment conditions employed for sample fabrication, the '700_1100' condition, denoting a calcination temperature of 700℃ and a sintering temperature of 1100℃, resulted in the most exceptional ionic conductivity of 4.89 × 10^-4 S/cm and a relative density of 88.72% for the LLZTO material. This is attributed to the low calcination temperature of 700℃, leading to reduced grain size and enhanced cohesiveness, thus resulting in a higher sintered density. In addition, a microstructure similar to the typical sintering characteristics observed in Spark Plasma Sintering (SPS) methods was identified in the SEM analysis results under the '700_1100' condition. Consequently, the '700_1100' heat treatment condition was deemed to optimal choice for enhancing ionic conductivity.

• 한국재료학회지
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• 제32권10호
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• pp.429-434
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• 2022

There is ongoing research to develop lithium ion batteries as sustainable energy sources. Because of safety problems, solid state batteries, where electrolytes are replaced with solids, are attracting attention. Sulfide electrolytes, with a high ion conductivity of 10^-3 S/cm or more, have the highest potential performance, but the price of the main materials is high. This study investigated lithium hydride materials, which offer economic advantages and low density. To analyze the change in ion conductivity in polymer electrolyte composites, PVDF, a representative polymer substance was used at a certain mass ratio. XRD, SEM, and BET were performed for metallurgical analyses of the materials, and ion conductivity was calculated through the EIS method. In addition, thermal conductivity was measured to analyze thermal stability, which is a major parameter of lithium ion batteries. As a result, the ion conductivity of LiH was found to be 10^-6 S/cm, and the ion conductivity further decreased as the PVDF ratio increased when the composite was formed.

• 한국분말재료학회지
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• 제29권6호
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• pp.485-491
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• 2022

Lithium lanthanum titanium oxide (LLTO) is a promising ceramic electrolyte because of its high ionic conductivity at room temperature, low electrical conductivity, and outstanding physical properties. Several routes for the synthesis of bulk LLTO are known, in particular, solid-state synthesis and sol-gel method. However, the extremely low ionic conductivity of LLTO at grain boundaries is one of the major problems for practical applications. To diminish the grain boundary effect, the structure of LLTO is tuned to nanoscale morphology with structures of different dimensionalities (0D spheres, and 1D tubes and wires); this strategy has great potential to enhance the ion conduction by intensifying Li diffusion and minimizing the grain boundary resistance. Therefore, in this work, 0D spherical LLTO is synthesized using ultrasonic spray pyrolysis (USP). The USP method primarily yields spherical particles from the droplets generated by ultrasonic waves passed through several heating zones. LLTO is synthesized using USP, and the effects of each precursor and their mechanisms as well as synthesis parameters are analyzed and discussed to optimize the synthesis. The phase structure of the obtained materials is analyzed using X-ray diffraction, and their morphology and particle size are analyzed using field-emission scanning electron microscopy.