• 한국세라믹학회지
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• 제56권2호
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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.

• 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.

• 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.

• 한국분말재료학회지
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• 제30권2호
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• pp.107-115
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• 2023

Li_1.3Al_0.3Ti_1.7(PO₄)₃(LATP) is considered a promising material for all-solid-state lithium batteries owing to its high moisture stability, wide potential window (~6 V), and relatively high ion conductivity (10^-3-10^-4 S/cm). Solid electrolytes based on LATP are manufactured via sintering, using LATP powder as the starting material. The properties of the starting materials depend on the synthesis conditions, which affect the microstructure and ionic conductivity of the solid electrolytes. In this study, we synthesize the LATP powder using sol-gel and co-precipitation methods and characterize the physical properties of powder, such as size, shape, and crystallinity. In addition, we have prepared a disc-shaped LATP solid electrolyte using LATP powder as the starting material. In addition, X-ray diffraction, scanning electron microscopy, and electrochemical impedance spectroscopic measurements are conducted to analyze the grain size, microstructures, and ion conduction properties. These results indicate that the synthesis conditions of the powder are a crucial factor in creating microstructures and affecting the conduction properties of lithium ions in solid electrolytes.

• Transactions on Electrical and Electronic Materials
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• 제15권2호
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• pp.96-99
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• 2014

We fabricated $(Li_{0.5-x}Na_xLa_{0.5})Ti_{0.8}Zr_{0.2}O_3$(LNTLZ)ceramics ($0{\leq}x{\leq}0.4$) with a perovskite structure via standard solid state synthesis. The influence of Na content on the structural and electrical properties of LNTLZ ceramics was also investigated. During XRD patterns analysis, all of the samples showed orthorhombic structure. The resistance of LNTLZ ceramics decreased as Na content increased, and the maximum activation energy shows 0.56 eV at x=0.4 at room temperature. These results indicated that LNTLZ ceramics are a candidate for use Lithium ion batteries as electrolytes.

• Journal of Electrochemical Science and Technology
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• 제12권1호
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• pp.126-136
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• 2021

The electrochemical performance of all-solid-state cells (ASSCs) based on sulfide electrolytes is critically affected by the undesirable interfacial reactions between oxide cathodes and sulfide electrolytes because of the high reactivity of sulfide electrolytes. Based on the concept that the interfacial reactions are highly dependent on the type of sulfide electrolyte, the electrochemical properties of the ASSCs prepared using three types of sulfide electrolytes were observed and compared. The Li2MoO4-LiI coating layer was also introduced to suppress the interfacial reactions. The cells using argyrodite electrolyte exhibited a higher capacity and Coulombic efficiency than the cells using 75Li2S-22P2S5-3Li2SO4 and Li7P3S11 electrolytes, indicating that the argyrodite electrolyte is less reactive with cathodes than other electrolytes. Moreover, the introduction of Li2MoO4-LiI coating on the cathode surface significantly enhanced the electrochemical performance of ASSCs because of the protection of coating layer. Pulverization of argyrodite electrolyte is also effective in increasing the capacity of cells because the smaller size of electrolyte particles improved the contact stability between the cathode and the sulfide electrolyte. The cyclic performance of cells was also enhanced by pulverized electrolyte, which is also associated with improved contact stability at the cathode/electrolyte. These results show that the introduction of Li2MoO4-LiI coating and the use of pulverized sulfide electrolyte can exhibit a synergic effect of suppressed interfacial reaction by the coating layer and improved contact stability owing to the small particle size of electrolyte.

• 전기화학회지
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• 제3권1호
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• pp.44-48
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• 2000

상온에서 DC-magnetron sputtering으로 증착한 비정질의 $V_2O_5$ 박막을 양극물질로 하여 $V_2O_5/LIPON/Li$으로 구성된 박막형 리튬이차전지를 제작하였다. $V_2O_5$의 양극특성은 액체전해질을 이용한 half cell 구조에서 평가하였으며, $Ar/O_2$ 분압비의 변화에 따라 제작된 $V_2O_5$ 양극은 분압비 80/20에서 가장 좋은 특성을 보였다. 자체 제작한 $Li_3PO_4$ 타겟을 사용하여 RF-sputtering으로 순수한 질소 분위기 하에서 양극 위에 고체전해질 LIPON 박막을 형성하였으며, 1.2-4.0V vs. Li 구간에서 리튬에 대해 반응성이 없는 안정한 화합물임을 확인하였다. 음극으로 쓰인 약 $2{\mu}m$두께의 금속리튬박막은 진공 열 증착법으로 제조하였으며, $V_2O_5/LIPON/Li$의 박막형 리튬이차전지는 $1.2\~3.5V$ 구간에서 초기에 약 $150{\mu}A/cm^2{\mu}m$의 높은 방전용량을 나타내었다.

• 전기화학회지
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• 제3권2호
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• pp.115-120
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• 2000

양극 물질로 산화바나듐 박막, 고체전해질로는 LiPON 박막 그리고 음극 물질로는 리튬 금속 박막을 선택하여 $Li/LiPON/V_2O_5/Pt$ 구조의 전고상 박막 전지를 제작하였고 전지 특성을 평가하였다. 산화바나듐 박막은 여러 산소 분압에서 직류 반응성 스퍼터링으로 증착하여 전기화학적 특성을 분석한 결과 $20\%\;O_2/Ar$비에서 가장 우수한 가역 특성을 나타내었다. 직류 반응성 스퍼터링에 의해 산화바나듐 박막을 제작한 후 진공을 그대로 유지한 상태에서 r.f. 반응성 스퍼터링에 의해 LiPON 고체전해질 박막을 증착하였다. 그 후 dry room내에서 진공 열증착법에 의해 리튬 금속 박막을 증착하여 전고상의 박막 전지를 제작하였다. $Li/LiPON/V_2O_5$ 박막 전지를 전압 범위와 전류 밀도를 변화시켜 충방전 시험을 행한 결과 $7{\mu}A/cm^2$의 전류 밀도와 3.6-2.7 V의 전압범위에서 가장 우수한 가역 특성을 나타내었다. $Li/LiPON/V_2O_5$박막 전지로 초시계를 구동 시켰으며 이는 in-situ공정에 의해 제작된 박막 전지가 소자 에너지원으로의 응용 가능성을 보여 주었다.

• 전기화학회지
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• 제11권2호
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• pp.100-104
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• 2008

Titanium sheet metal substrates used in thin film batteries were wet etched and their surface area was increased in order to increase the discharge capacity and power density of the batteries. To obtain a homogeneous etching pattern, we used a conventional photolithographic process. Homogeneous hemisphere-shaped wells with a diameter of approximately $40\;{\mu}m$ were formed on the surface of the Ti substrate using a photo-etching process with a $20\;{\mu}m{\times}20\;{\mu}m$ square patterned photo mask. All-solid-state thin film cells composed of a Li/Lithium phosphorous oxynitride (Lipon)/$LiCoO_2$ system were fabricated onto the wet etched substrate using a physical vapor deposition method and their performances were compared with those of the cells on a bare substrate. It was found that the discharge capacity of the cells fabricated on wet etched Ti substrate increased by ca. 25% compared to that of the cell fabricated on bare one. High discharge rate was also able to be obtained through the reduction in the internal resistance. However, the cells fabricated on the wet etched substrate exhibited a higher degradation rate with charge-discharge cycling due to the nonuniform step coverage of the thin films, while the cells on the bare substrate demonstrated a good cycling performance.

• 전기화학회지
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• 제3권4호
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• pp.219-223
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• 2000

구리-바나듐 산화물 양극을 이용하여 $(Cu_{0.5}V_2O_5)$으로 구성된 전 고상의 리튬이차박막전지를 제작하였다. 구리-바나듐 산화물 박막은 reactive DC magnetron sputtering을 이용하여 co-sputtering에 의해 제조하였고 Lipon고체전해질은 순수한 질소 분위기 하에서 RF 스퍼터링으로 제조하였다. XRD분석을 통해 구리-바나듐 산화물 박막이 비정질임을 확인하였고, EC:DMC(1:1 in IM $LiPF_5$)액체전해질을 사용한 반전지 구조에서 그 전기화학적 특성을 고찰하였다. Lipon고체전해질의 이온전도도는 $25^{\circ}C$에서 $1.02\times10^{-6}S/cm$를 나타내었고 전고상 박막전지는 $1.5V\~3.6V$의 전압구간, $50{\mu}A/cm^2$의 전류밀도에서 500싸이클까지 약 $50{\mu}Ah/cm^2{\mu}m$의 방전용량을 유지하였다