• Journal of the Korean institute of surface engineering
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• v.39 no.6
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• pp.255-262
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• 2006

Pd-Cu alloy membrane for hydrogen separation was fabricated by sputtering and Cu reflow process. At first, the Pd and Cu was continuously deposited by sputtering method on oxidized Si support, the Cu reflow process was followed. Microstructure of the surface and permeability of the membrane was investigated depending on various reflow temperature, time, Pd/cu composition and supports. With respect to our result, Pd-Cu thin film (90 wt.% Pd/10 wt.% Cu) deposited by sputtering process with thickness of $2{\mu}m$ was heat-treated for Cu reflow The voids of the membrane surface were completely filled and the dense crystal surface was formed by Cu reflow behavior at $700^{\circ}C$ for 1 hour. Cu reflow process, which is adopted for our work, could be applied to fabrication of dense Pd-alloy membrane for hydrogen separation regardless of supports. Ceramic or metal support could be easily used for the membrane fabricated by reflow process. The Cu reflow process must result in void-free surface and dense crystalline of Pd-alloy membrane, which is responsible for improved selectivity oi the membrane.

• Journal of the Korean Ceramic Society
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• v.49 no.6
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• pp.648-653
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• 2012

Hybridization of dense ceramic membranes for hydrogen separation with an electronically conductive metallic phase is normally utilized to enhance the hydrogen permeation flux and thereby to increase the production efficiency of hydrogen. In this study, we developed a nickel and proton conducting oxide ($BaCe_{0.9}Y_{0.1}O_{3-{\delta}}$: BCY) based cermet (ceramic-metal composites) membrane. Focused on the general criteria in that the hydrogen permeation properties of a cermet membrane depend on its microstructural features, such as the grain size and the homogeneity of the mix, we tried to optimize the microstructure of Ni-BCY cermets by controlling the fabrication condition. The Ni-BCY composite powder was synthesized via a solid-state reaction using $2NiCO_3{\cdot}3Ni(OH)_2{\cdot}4H_2O$, $BaCeO_3$, $CeO_2$ and $Y_2O_3$ as a starting material. To optimize the mixing scale and homogeneity of the composite powder, we employed a high-energy milling process. With this high-energy milled composite powder, we could fabricate a fine-grained dense membrane with an excellent level of mixing homogeneity. This controlled Ni-BCY cermet membrane showed higher hydrogen permeability compared to uncontrolled Ni-BCY cermets created with a conventionally ball-milled composite powder.

• Proceedings of the Membrane Society of Korea Conference
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• 2002.05a
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• pp.35-41
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• 2002

Dense oxygen ionic conducting materials can be used for oxygen separation membranes at high temperatures. However, they show relatively low permeation flux because of their large resistances. To reduce resistances and improve the oxygen permeation flux, thin dense yttria-stabilized-zirconia (YSZ)/Pd composite dual-phase membranes were fabricated by a new approach that combines the reservoir method and chemical vapor deposition (CVD). A thin porous YSZ layer was coated on a porous alumina support by dip-coating the YSZ suspension. A continuous Pd phase was formed inside pores of the YSZ layer by the reservoir method. The residual pores of the YSZ/Pd layer were plugged with yttria/zirconia by CVD to ensure the gas tightness of the membranes. The oxygen permeation fluxes through these composite membrane were 2.0$\times$10$^{-8}$ mol/cm$^2$.s and 4.8$\times$10$^{-8}$ mol/cm$^2$.s at 105$0^{\circ}C$ when air and oxygen were used as the permeate gases, respectively. These oxygen permeation values are about 1 order of magnitude higher than those of pure YSZ membranes prepared under similar conditions.

• Journal of the Korean Crystal Growth and Crystal Technology
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• v.22 no.1
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• pp.19-24
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• 2012

Barium zirconate exhibits good thermo-chemical stability and proton conduction at high temperatures, but shows poor electron conductivity. Therefore, for high efficiency of hydrogen separation, a very thin and dense Pd-Barium zirconate membrane has to be coated on a porous substrate. A thin and dense Pd-Barium zirconate membrane was successfully synthesized on a porous substrate by means of dual sputtering method. The structural and chemical features of the $BaZr_{0.85}Y_{0.15}O_{3-{\delta}}$ membranes sputtered at $300^{\circ}C$ and $400^{\circ}C$ were investigated by X-ray diffractometry, and it was found that a well-crystallized membrane, Pm-3m space group of $BaZrO_3$, was synthesized. The surface and cross-sectional morphologies of membrane were assessed by SEM (scanning electron microscopy) and TEM(transmission electron microscopy) of the surface and of cross sections. The cross sectional observation of Pd-$BaZr_{0.85}Y_{0.15}O_{3-{\delta}}$ membrane by dual sputtering shows that the coating is quite dense with columnar structure.

• Transactions of the Korean hydrogen and new energy society
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• v.21 no.2
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• pp.117-122
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• 2010

BCY($Ba(Ce_{0.9}Y_{0.1})O_{3-\delta}$) oxide, shows high protonic conductivity at high temperatures, and are referred to as hydrogen separation membrane. For high efficiency of hydrogen separation ($H_2$ flux and selectivity) and low fabrication cost, ultimate thin and dense BCY-Ni layer have to be coated on a porous substrate such as $ZrO_2$. Aerosol depostion (AD) process is a novel technique to grow ceramic film with high density and nano-crystal structure at room-temperature, and would be applied to the fabrication process of AD integration ceramic layer effectively. XRD and SEM measurements were conducted in order to analyze the characteristics of BCY-Ni membrane fabricated by AD process.

• Korean Membrane Journal
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• v.9 no.1
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• pp.34-42
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• 2007

A perovskite-type ($La_{0.6}Sr_{0.4}Ti_{0.2}Fe_{0.8}O_{3-{\delta}}$) dense ceramic membrane was prepared by polymerized complex method, using citric acid as a chelating agent and ethylene glycol as an organic stabilizer. Effect of Ti addition on lanthanum-strontium ferrite mixed conductor was investigated by evaluating the thermal expansion coefficient, the oxygen flux, the electrical conductivity, and the phase stability. The thermal expansion coefficient in air was $21.19\;{\times}\;10^{-6}/K$ at 473 to 1,223 K. At the oxygen partial pressure of 0.21 atm ($20%\;O_2$), the electrical conductivity increased with temperature and then decreased after 973 K. The decrement in electrical conductivity at high temperatures was explained by a loss of the lattice oxygen. The oxygen flux increased with temperature and was $0.17\;mL/cm^2{\cdot}min$ at 1,223 K. From the temperature-dependent oxygen flux data, the activation energy of oxygen ion conduction was calculated and was 80.5 kJ/mol at 1,073 to 1,223 K. Also, the Ti-added lanthanum-strontium ferrite mixed conductor was structurally and chemically stable after 450 hours long-term test at 1,173 K.

• Transactions of the Korean hydrogen and new energy society
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• v.21 no.4
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• pp.271-277
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• 2010

$(Ba(Zr_{0.85}Y_{0.15})O_{3-\delta})$ oxide, showing high protonic conductivity at high temperatures and good chemical stability with $CO_2$ are referred to as hydrogen separation membrane. For high efficiency of hydrogen separation ($H_2$ flux and selectivity) and low fabrication cost, ultimate thin and dense BZY-Ni layer has to be coated on a porous substrate such as $ZrO_2$. Aerosol depostion (AD) process is a novel technique to grow ceramic film with high density and nano-crystal structure at room-temperature, and may be applicable to the fabrication process of AD integration ceramic layer effectively. XRD, SEM, X-ray mapping measurements were conducted in order to analyze the characteristics of BZY-Ni membrane fabricated by AD process. it is observed that it is homogeneous distribution for BZY-Ni. The result of $H_2$ permeation rate suggests that BZY-Ni composite is higher than BZY.

• Journal of the Korean Ceramic Society
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• v.44 no.1 s.296
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• pp.58-64
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• 2007

In this study, we investigated $Li_2ZrO_3$ membrane as a candidate material for high-temperature $CO_2$ separation and evaluated mechanical property. $Li_2ZrO_3$ powder was synthesized by solid state reaction of $Li_2CO_3\;and\;ZrO_2$. Then we fabricated $Li_2ZrO_3$ tape using tape casting method. Dense $Li_2ZrO_3$ membrane prepared by sintering at $1600^{\circ}C$ for 2 h after pressing $Li_2ZrO_3$ tape using lamination machine. Mechanical properties before and after $CO_2$ absorption of fabricated $Li_2ZrO_3$ membrane such as Hertzian indentation, Victors hardness and 3-point bending testing were evaluated.

• Membrane Journal
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• v.21 no.4
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• pp.321-328
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• 2011

$PrBa_{0.9}Sr_{0.1}Co_2O_{5+{\delta}}$ oxide was synthesized by soild state reaction method. Dense ceramic membrane was prepared using as-prepared powder by pressing and sintering at $1250^{\circ}C$. XRD result of membrane showed double perovskite structure. Leakage and oxygen permeation test were conducted on the membrane sealed by pyrex ring as a sealing material. Oxygen permeation was measured in the temperature range from 850 to $950^{\circ}C$. The oxygen flux of $PrBa_{0.9}Sr_{0.1}Co_2O_{5+{\delta}}$ membrane was increased with the temperature from 0.15 to $0.32mL/cm^2{\cdot}min$.

• Transactions of the Korean hydrogen and new energy society
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• v.21 no.4
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• pp.264-270
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• 2010

Recently, the most promising methods for high purity hydrogen production are membranes separation such as polymer, metal, ceramic and composites. It is well known that Pd and Pd-alloys membranes have excellent properties for hydrogen separation. However, it has hydrogen embrittlement and high cost for practical applications. Therefore, most scientists have studied new materials instead of Pd and Pd-alloys. On the other hand, TiN powders are great in resistance to acids and chemically stable under high operating temperature. In order to get specimens for hydrogen permeation, the TiN powders synthesized were consolidated together with Co, Ni powders by hot press sintering (HPS). During the consolidation of powders at HPS, heating rate was 10 K/min and the pressure was 10 MPa. It was characterized by XRD, SEM. Also, we estimated the hydrogen permeability by Sievert's type hydrogen permeation membrane equipment.