• Membrane Journal
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• v.32 no.6
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• pp.456-464
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• 2022

Hydrogen permeation performance was analyzed by manufacturing Pd and Pd-Cu membranes through electroless plating. As a support for the Pd and Pd-Cu membranes, α-Al₂O₃ ceramic hollow fiber were used. Pd-Cu membrane was manufactured through sequential electroless plating, and then annealing was performed at 500°C, for 18 h in a hydrogen atmosphere to make Pd and Cu alloy. After annealing, the Pd-Cu membrane confirmed that the alloy was formed through EDS (Energy Dispersive X-ray Spectroscopy) and XRD (X-ray Diffraction) analysis. In addition, the thickness of the Pd and Pd-Cu plating layers were measured to be about 3.21 and 3.72 µm, respectively, through SEM (Scanning Electron Microscope) analysis. Hydrogen permeation performance was tested for hydrogen permeation in the range of 350~450°C and 1~4 bar in hydrogen single gas and mixed gas (H₂, N₂). In a single hydrogen gas, Pd and Pd-Cu membranes have flux of up to 54.42 and 67.17 ml/cm²⋅ min at 450 °C and 4 bar. In the mixed gas, it was confirmed that the separation factors of 1308 and 453 were obtained under the conditions of 450 °C and 4 bar.

• Proceedings of the Membrane Society of Korea Conference
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• 1999.07a
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• pp.111-113
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• 1999

• Journal of the Korean institute of surface engineering
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• v.45 no.6
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• pp.248-256
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• 2012

A Pd-based hydrogen membranes for hydrogen purification and separation need high hydrogen perm-selectivity. The surface roughness of the support is important to coat the pinholes free and thin-film membrane over it. Also, The pinholes drastically decreased the hydrogen perm-selectivity of the Pd-based composite membrane. In order to remove the pinholes, we introduced various surface pre-treatment such as alumina powder packing, nickel electro-plating and micro-polishing pre-treatment. Especially, the micro-polishing pretreatment was very effective in roughness leveling off the surface of the porous nickel support, and it almost completely plugged the pores. Fine Ni particles filled surface pinholes with could form open structure at the interface of Pd alloy coating and Ni support by their diffusion to the membrane and resintering. In this study, a $4{\mu}m$ surface pore-free Pd-Cu-Ni ternary alloy membrane on a porous nickel substrate was successfully prepared by micro-polishing, high temperature sputtering and Cu-reflow process. And $H_2$ permeation and $N_2$ leak tests showed that the Pd-Cu-Ni ternary alloy hydrogen membrane achieved both high permeability of $13.2ml{\cdot}cm^{-2}{\cdot}min^{-1}{\cdot}atm^{-1}$ permation flux and infinite selectivity.

• Applied Chemistry for Engineering
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• v.17 no.5
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• pp.458-464
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• 2006

The Pd-Ni-Ag alloy composite membrane using modified porous stainless steel (PSS) as a substrate was prepared by a electroless plating technique. In this work, we have introduced the intermediate layer between Pd-based alloy and a metal substrate. As an intermediate layer, the mixtures of nickel powder and inorganic sol such as $SiO_{2}$ sol, $Al_{2}O_{3}$ sol, and $TiO_{2}$ sol were used. The intermediate layers were coated onto a PSS substrate according to various membrane preparation conditions and then $N_{2}$ fluxes through the membranes with different intermediate layers were measured. The surface morphology of the intermediate layer in the mixture of nickel powder and inorganic sol was analyzed using scanning electron microscope (SEM). Finally, the Pd-Ni-Ag alloy composite membrane using the support coated with the mixture of nickel powder and silica as an intermediate layer was fabricated and then the gas permeances for $H_{2}$ and $N_{2}$ through the Pd-based membrane were investigated. The selectivity of $H_2/N_2$ was infinite and the $H_{2}$ flux was $1.39{\times}10^{-2}mol/m^2{\cdot}s$ at the temperature of $500^{\circ}C$ and trans-membrane pressure difference of 1 bar.

• 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.

• Membrane Journal
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• v.21 no.2
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• pp.148-154
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• 2011

Metal-ceramic composite membrane have been developed to separate hydrogen from mixed gases, particularly product streams generated during coal gasification and methane reforming. Cermet membrane was fabricated with palladium as hydrogen-permeable metal and $Y_2O_3$-stabilized $ZrO_2$ (YSZ) as ceramic supporter. As-prepared membrane showed dense structure with continuous channel of palladium. The hydrogen flux of Pd/YSZ membrane have been measured in the range of 0.5~2 atm with 100% hydrogen gas. The results indicate that the hydrogen flux was 0.333 mL/$min{\cdot}cm^2$ at $450^{\circ}C$ and 2 atm. The crack was formed in the surface and cross-section of membrane.

• Corrosion Science and Technology
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• v.6 no.3
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• pp.133-139
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• 2007

Nickel powder was coated with aluminum nitrate solution to increase the thermal stability of a porous nickel support and control the nickel content in the Pd-Cu-Ni ternary alloyed membrane. Raw nickel powder and alumina coated nickel powder were uniaxialy pressed by home made press with metal cylindrical mold. Though the used nickel powder prepared by pulsed wire evaporation (PWE) method has a good thermal stability, the porous nickel support was too much sintered and the pores of porous nickel support was plugged at high temperature (over $800^{\circ}C$) making it not suitable for the porous support of a palladium based composite membrane. In order to overcome this problem, the nickel powder was coated by alumina and alumina modified porous nickel support resists up to $1000^{\circ}C$ without pore destruction. Furthermore, the compositions of Pd-Cu-Ni ternary alloy membrane prepared by magnetron sputtering and Cu-reflow could be controlled by not only Cu-reflow temperature but also alumina coating amount. SEM analysis and mercury porosimeter analysis evidenced that the alumina coated on the surface of nickel powder interrupted nickel sintering.

• Applied Chemistry for Engineering
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• v.29 no.2
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• pp.196-200
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• 2018

In this study, the intermediate layer in Pd-based hydrogen separation membrane was synthesized to minimize the surface roughness and defects using powder-type and sol-type metal oxides. The surface properties and gas permeation characteristics were analysed by SEM and $N_2$ gas permeation test. The coating layer composed of sol type metal oxides has smooth surface, especially the layer coated by $TiO_2$ sol has little pin holes, cracks and defects. The binary layer composed of powder type and sol type metal oxides has similar flux characteristics to a single sol type layer. The Pd-based composite membrane improved by the binary intermediate layer exhibited $0.32mol/m^2s$ of the hydrogen permeation flux with a selectivity ($H_2/N_2$) of ~10,890 at 672 K and a pressure difference of 1 bar.

• Korean Chemical Engineering Research
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• v.44 no.2
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• pp.160-165
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• 2006

A Pd-Cu-Ni alloyed hydrogen membrane has fabricated on porous nickel support formed by nickel powder. Porous nickel support made by sintering shows a strong resistance to hydrogen embrittlement and thermal fatigue. Plasma surface modification treatment is introduced as pre-treatment process instead of conventional HCl wet activation. Nickel was electroplated to a thickness of $2{\mu}m$ in order in to fill micropores at the nickel support surface. Palladium and copper were deposited at thicknesses of $4{\mu}m$ and $0.5{\mu}m$, respectively, on the nickel coated support by DC sputtering process. Subsequently, copper reflow at $700^{\circ}C$ was performed for an hour in $H_2$ ambient. And, as a result PdCu-Ni composite membrane has a pinhole-free and extremely dense microstructure, having a good adhesion to the porous nickel support and infinite hydrogen selectivity in $H_2/N_2$ mixtures.