• Journal of the Korean Ceramic Society
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• v.56 no.2
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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.

• Journal of the Microelectronics and Packaging Society
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• v.10 no.2
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• pp.49-54
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• 2003

We have investigated the effects of hydrogen annealing on the physical and electrical properties of $SrBi_{2}Ta_{2}O_9(SBT)$ thin films in the Pt/SBT/Si (MFS) structure and Pt/SBT/Pt (MFM) one, respectively. The microstructure and electrical characteristics of the SBT films were deteriorated after hydrogen annealing due to the damage of the SBT films during the annealing process. To investigate the reason of the degradation of the SBT films in this work, in particular, the effect of the Pt top electrodes, SBT thin films deposited on Si, Pt, respectively, were annealed with the same process conditions. From the XRD, XPS, P-V, and C-V data, it was seen that the SBT itself was degraded after $H_2$ annealing even without the Pt top electrodes. In addition, the degradation of the SBT films after $H_2$ annealing was accelerated by the catalytic reaction of the Pt top electrodes which is so-called hydrogen degradation. To prevent this phenomenon, we proposed the alternative top electrode material, i.e. Ir, and the electrical properties of the SBT thin films were examined in the $Ir/IrO_2/SBT/IrO_2$ structures before and after the H$_2$ annealing and recovery heat-treatment processes. From the results of the P-V measurement, it could be concluded that Ir is one of the promising candidate as the electrode material for degradation resistance in the MFM structure using SBT thin films.

• Proceedings of the Korean Vacuum Society Conference
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• 2012.02a
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• pp.250-250
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• 2012

Recently, multiferroic materials have attracted much attention due to their fascinating fundamental physical properties and potential technological applications in magnetic/ferroelectric data storage systems, quantum electromagnets, spintronics, and sensor devices. Among single-phase multiferroic materials, $BiFeO_3$, in particular, has received considerable attention because of its very interesting magnetoelectric properties for application to spintronics. Enhanced ferromagnetism was found by Fe-site ion substitution with magnetic ions. In this study, $BiFe_{1-x}Ni_xO_3$ (x=0 and 0.05) bulk ceramic compounds were prepared by solid-state reaction and rapid sintering. High-purity $Bi_2O_3$, $Fe_3O_4$ and NiO powders were mixed with the stoichiometric proportions, and calcined at $450^{\circ}C$ for 24 h to produce $BiFe_{1-x}Ni_xO_3$. Then, the samples were directly put into the oven, which was heated up to $800^{\circ}C$ and sintered in air for 20 min. The crystalline structure of samples was investigated at room temperature by using a Rigaku Miniflex powder diffractometer. The Raman measurements were carried out with a Raman spectrometer with 514.5-nm-excitation Ar+-laser source under air ambient condition on a focused area of $1-{\mu}m$ diameter. The field-dependent magnetization and the temperature-dependent magnetization measurements were performed with a vibrating-sample magnetometer. The x-ray diffraction study demonstrates the compressive stress due to Ni substitution at the Fe site. $BiFe_{0.95}Ni_{0.05}O_3$ exhibits the rhombohedral perovskite structure R3c, similar to $BiFeO_3$. The lattice constant of $BiFe_{0.95}Ni_{0.05}O_3$ is smaller than of $BiFeO_3$ because of the smaller ionic radius of Ni3+ than that of Fe3+. The field-dependent magnetization of $BiFe_{0.95}Ni_{0.05}O_3$ exhibits a clear hysteresis loop at 300 K. The magnetic properties of $BiFe_{0.95}Ni_{0.05}O_3$ were improved at room temperature because of the existence of structurally compressive stress.

• Journal of the Microelectronics and Packaging Society
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• v.26 no.4
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• pp.127-132
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• 2019

In this study, barium strontium titanate (BSTO) with high dielectric perovskite structure was synthesized by liquid-solid solution synthesis and the surface was modified using trimethylsilyl chloride (TMCS) as a silylation agent. Silylation surface modification is a method of reacting -OH ligand on the surface of BSTO nanoparticles with Cl in TMCS to generate HCl and replacing the ligand on the surface of nanoparticles with -Si, -CH₃. Silylation was optimized by varying the concentration of TMCS, and the structure of the silicon network was confirmed by Fourier-transform infrared spectroscopy. In addition, the crystallinity of BSTO nanoparticles was confirmed by X-ray diffractometer and the size of the nanoparticles was calculated using Scherrer equation. The field emission scanning electron microscopic image observed the change of the surface-modified BSTO particle size, and the contact angle measurement confirmed the hydrophobic property of the contact angle of 120.9° in the optimized nanoparticles. Finally, the surface-modified BSTO dispersion experiment in de-ionized water confirmed the hydrophobic degree of the nanoparticles.

• Journal of the Korean Electrochemical Society
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• v.1 no.1
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• pp.1-7
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• 1998

For the purpose of finding new cathode materials for medium-temperature $(700\~800^{\circ}C)$ solid oxide fuel cells, $Gd_{0.8}Ca_{0.2}Co_{1-x}Fe_xO_3,\;(x=0.0\~0.5)$ are prepared, and their thermal stability and conductivity characteristics are investigated. Also, the cathodic activities are measured after the cathode layer being attached on CGO (cerium-gadolinium oxide) electrolyte disk. The X-ray analyses indicate that the materials prepared by calcining the citrate-gels at $800^{\circ}C$ have the orthorhombic perovskite structure without discernible impurities. The thermal stability of the undoped Co perovskite is so poor that it is decomposed to the individual binary oxide even at $1300^{\circ}C$. But the partially Fe-doped cobaltates exhibit a better thermal stability to retain their structural integrity up to $1400^{\circ}C$. The observation whereby both the undoped and Fe-doped cobaltates melt at ca. $1300^{\circ}C$ leads us to perform the electrode adhesion at <$1300^{\circ}C$. The cathodic activity of $Gd_{0.8}Ca_{0.2}Co_{1-x}Fe_xO_3,\;(x=0.0\~0.5)$, electrodes is superior to $La_{0.9}Sr_{0.1}MnO_3$, among the samples of $x=0.0\~0.5$, the x=0.2 cathode shows the best activity for the oxygen reduction reaction. It is likely that the Fe-doping provides a better thermal stability to the materials but in turn imparts an inferior cathodic activity, such that the optimum trade-off is made at x=0.2 between the two factors. The total electrical conductivity and ion conductivity of $Gd_{0.8}Ca_{0.2}Co_{1-x}Fe_xO_3$, are measured to be 51 S/cm and $6.0\times10^{-4}S/cm\;at\;800^{\circ}C$, respectively. The conductivity values illustrate that the materials are a mixed conductor and the reaction sites can be expanded to the overall electrode surface, thereby providing a better cathodic activity than $La_{0.9}Sr_{0.1}MnO_3$.

• Journal of the Institute of Electronics Engineers of Korea SD
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• v.39 no.3
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• pp.1-8
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• 2002

In order to study electric properties of (Pb$\_$0.9/La$\_$0.1/)Ti$\_$0.975/O$_3$(PLT (10)) films with varying excess lead concentration (7.5, 10, 12.5, 15 ㏖% excess lead), the PLT films were deposited by sol-gel process. DTA analyses reveal that the crystallization temperature of the precursor powers decreased with increasing amount of excess lead. XRD patterns of PLT reveal pure perovskite structure and the preferred orientation increased with increasing Pb content in the films. With increasing amount of excess P$\_$b/, the relative permittivity ($\xi$$\_$r/) increased and leakage current density at 100 ㎸/cm transformed 4.01$\times$10$\^$-5/, 2.42$\times$10$\^$-6/, 1.27$\times$10$\^$-6/, 1.56$\times$10$\^$-6/A/㎠ respectively. In the results of hysteresis loops measured at 166 kV/cm, the remanent polarization (P$\_$r/) and the coercive field (E$\_$c) are 6.36$\mu$C/cm and 58.7 ㎸/cm, respectively (at 12.5 ㏖% excess P$\_$b/) With increasing amount of excess Pb, the remanent polarization for PLT thin film degraded to about 44%, 27%, 15%, 16% of the initial value after 10$\^$9/ cycles./TEX>) With increasing amount of excess Pb, the remanent polarization for PLT thin film degraded to about 44%, 27%, 15%, 16% of the initial value after $10^{9}$ cycles.

• Journal of the Korean Ceramic Society
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• v.40 no.4
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• pp.323-327
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• 2003

Microwave dielectric properties of (P $b_{0.4}$C $a_{0.6}$)[($Fe_{\frac{1}{2}}$N $b_{\frac{1}{2}}$)$_{1-x}$ (M $g_{1}$ 3/N $b_{2}$ 3/)x] $O_3$ (PCFMN) ceramics were investigated as a function of (M $g_{1}$ 3/N $b_{2}$ 3/)$^{4+}$ content (0.1$\leq$x$\leq$0.8). A single perovskite phase with the cubic structure was obtained through the given composition range. The unit cell volume was increased with (M $g_{1}$ 3/N $b_{2}$ 3/)$^{4+}$, due to the larger average ionic size of (M $g_{1}$ 3/N $b_{2}$ 3/)$^{4+}$ than that of ($Fe_{\frac{1}{2}}$N $b_{\frac{1}{2}}$)$^{4+}$ for B-site ion. Dielectric constant (K) and Temperature Coefficient of Resonant Frequency(TCF) of PCFMN ceramics were dependent on (M $g_{1}$ 3/N $b_{2}$ 3/)$^{4+}$ content due to the decrease of ionic polarizability and B-site bond valence, respectively. Qf value was decreased with (M $g_{1}$ 3/N $b_{2}$ 3/)$^{4+}$ content due to the decrease of grain size. Typically, K of 73.56, Qf of 5,074 GHz and TCF of -6.45 ppm/$^{\circ}C$ were obtained for the specimens with x=0.4 sintered at 125$0^{\circ}C$ for 3 h.125$0^{\circ}C$ for 3 h.

• Korean Journal of Materials Research
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• v.20 no.11
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• pp.575-580
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• 2010

The microstructure and positive temperature coefficient of resistivity (PTCR) characteristics of 0.1 mol%$Na_2Ti_6O_{13}$ doped $0.94BaTiO_3-0.06(Bi_{0.5}Na_{0.5})TiO_3$ (BBNT-NT001) ceramics sintered at various temperatures from $1200^{\circ}C$ to $1350^{\circ}C$ were investigated in order to develop eco-friendly PTCR thermistors with a high Curie temperature ($T_C$). Resulting thermistors showed a perovskite structure with a tetragonal symmetry. When sintered at $1200^{\circ}C$, the specimen had a uniform microstructure with small grains. However, abnormally grown grains started to appear at $1250^{\circ}C$ and a homogeneous microstructure with large grains was exhibited when the sintering temperature reached $1325^{\circ}C$. When the temperature exceeded $1325^{\circ}C$, the grain growth was inhibited due to the numerous nucleation sites generated at the extremely high temperature. It is considered that $Na_2Ti_6O_{13}$ is responsible for the grain growth of the $0.94BaTiO_3-0.06(Bi_{0.5}Na_{0.5})TiO_3$) ceramics by forming a liquid phase during the sintering at around $1300^{\circ}C$. The grain growth of the BBNT-NT001 ceramics was significantly correlated with a decrease of resistivity. All the specimens were observed to have PTCR characteristics except for the sample sintered at $1200^{\circ}C$. The BBNT-NT001 ceramics had significantly decreased $\tilde{n}_{rt}$ and increased resistivity jump with increasing sintering temperature at from $1200^{\circ}C$ to $1325^{\circ}C$. Especially, the BBNT-NT001 ceramics sintered at $1325^{\circ}C$ exhibited superior PTCR characteristics of low resistivity at room temperature ($122\;{\Omega}{\cdot}cm$), high resistivity jump ($1.28{\times}10^4$), high resistivity temperature factor (20.4%/$^{\circ}C$), and a high Tc of $157.9^{\circ}C$.

• Membrane Journal
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• v.21 no.2
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• pp.155-162
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• 2011

Dense tubular $Ba_{0.5}Sr_{0.5}Co_{0.8}Fe_{0.2}O_{3-{\delta}}$ (BSCF) membranes were prepared by extrusion technique. The phase structure of the $Ba_{0.5}Sr_{0.5}Co_{0.8}Fe_{0.2}O_{3-{\delta}}$ membranes was characterized by X-ray diffraction (XRD) and scanning electron microscope (SEM). Relative density of $Ba_{0.5}Sr_{0.5}Co_{0.8}Fe_{0.2}O_{3-{\delta}}$ tubular membrane was 94.10%. Oxygen permeation was measured at difference operating condition of feed side and permeate side in the temperature range from 700 to $950^{\circ}C$. The oxygen permeation flux of dense tubular $Ba_{0.5}Sr_{0.5}Co_{0.8}Fe_{0.2}O_{3-{\delta}}$ membrane reached maximum 1.37 mL/$min{\cdot}cm^2$ at $900^{\circ}C$ exposed to ambient air (feed side) and vacuum pump (permeate side).

• Journal of the Korean Institute of Electrical and Electronic Material Engineers
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• v.23 no.12
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• pp.929-935
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• 2010

$(1-x)BaTiO_3-x(Bi_{0.5}Na_{0.5})TiO_3$ ($0.01{\leq}x{\leq}0.10$) ceramics were fabricated with muffled sintering by a modified synthesis process. Their positive temperature coefficient of resistivity (PTCR) characteristics were investigated systematically. All specimen showed a perovskite structure with a tetragonal symmetry. Both the lattice parameter of a and c axes were slightly decreased with increasing $(Bi_{0.5}Na_{0.5})TiO_3$ (BNT) content. Grain growth was achieved when the incorporated BNT was increased to 6 mol% and the inhibition of grain growth is considered to be due to the appearance of Ba vacancy ($V^{"}_{Ba}$) in the $(1-x)BaTiO_3-x(Bi_{0.5}Na_{0.5})TiO_3$ ($0.08{\leq}x$). With 4 mol% BNT addition, room temperature resistivity decreased to $48 \Omega{\cdot}cm$ and a resistivity jump ($\rho_{max}/\rho_{min}$) was as high as $1.1{\times}10^4$, respectively. Curie temperature was also increased to $171^{\circ}C$ with increasing BNT content.