# US 9,751,051 B2 · Hydrogen separation membrane, and method for manufacturing same

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- Number: US 9,751,051 B2
- Document ID: US9751051B2
- Status: Granted
- Kind: B2
- Application number: 14/651,596
- Filed: 2013-10-31
- Published: 2015-11-19
- Granted: 2017-09-05
- Earliest claimed: 2012-12-11
- Assignees: Korea Institute of Energy Research
- Applicants: Korea Institute of Energy Research
- Inventors: Jongsoo Park; Shinkun Ryi; Chunboo Lee; Sungwook Lee
- Web page: https://patentgrep.com/patent/US9751051B2

## CPC

- B01D 69/108: {Inorganic support material}
- B01D 53/228: {characterised by specific membranes}
- B01D 63/081: {Manufacturing thereof}
- B01D 67/0072: {by deposition from the gaseous phase, e.g. sputtering, CVD, PVD}
- B01D 71/0221: {Group 4 or 5 metals}
- B01D 71/02231: {Palladium}
- B01D 71/02232: {Nickel}
- B01D 71/024: {Oxides}
- C01B 3/505: Membranes containing palladium
- C23C 8/10: Oxidising
- C23C 14/34: Sputtering
- B01D 2257/108: Hydrogen
- B01D 2325/20: Specific permeability or cut-off range
- B01D 2325/28: Degradation or stability over time
- B01D: SEPARATION (separating solids from solids by wet methods B03B, B03D; by pneumatic jigs or tables B03B; by other dry methods B07; magnetic or electrostatic separation of solid materials from solid materials or fluids, separation by high-voltage electric fields B03C; centrifuges, vortex apparatus B04; presses per se for squeezing-out liquid from liquid-containing material B30B9/02; treatment of water C02F, e.g. softening by ion-exchange C02F1/42; {arrangements of air intake cleaners in gas turbine plants F02C7/05} ; arrangements or mounting of filters in air-conditioning, air-humidification or ventilation F24F13/28)
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- C23C: COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL (making metal-coated products by extrusion B21C23/22; covering with metal by connecting pre-existing layers to articles, see the relevant places, e.g. B21D39/00, B23K; metallising of glass C03C; metallising mortars, concrete, artificial stone, ceramics or natural stone C04B41/00; enamelling of, or applying a vitreous layer to, metals C23D; treating metal surfaces or coating of metals by electrolysis or electrophoresis C25D; single-crystal film growth C30B; by metallising textiles D06M11/83; decorating textiles by locally metallising D06Q1/04)

## Abstract

The present invention relates to a hydrogen separation membrane and to a method for manufacturing same, which is provided for restraining the diffusion of and for imparting excellent bonding characteristics between a porous support and a palladium-based metal separation membrane. The hydrogen separation membrane according to the present invention comprises: a porous support of a metal material or a ceramic material; a buffer layer formed as a plurality of columns by using a ceramic material on the porous support; and a palladium-based metal separation membrane formed on the buffer layer for separating hydrogen. In said case, the buffer layer includes an oxide-based ceramic material of either MOy (M is Ti, Zr), wherein which the composition of oxygen is 1<y<2, or Al2Oz, wherein which the composition of oxygen is 2<z<3, and may be formed as a plurality of layers.

## Claims

### Claim 1

A hydrogen separation membrane comprising:
a porous support made of a metal or ceramic material;
a buffer layer made of a ceramic material, and formed in the form of a plurality of columns on the porous support, wherein the buffer layer is formed of a plurality of layers; and
a palladium-based metal separation membrane formed on the buffer layer and capable of separating hydrogen,
wherein the buffer layer has neighboring layers formed of different ceramic materials, the buffer layer comprises:
a first buffer layer formed on the porous support, and formed of one oxide-based ceramic material selected from the group consisting of TiOy, ZrOy, and Al2Oz where the composition of oxygen is 1<y<1.8, or 2<z<2.8; and
a second buffer layer formed on the first buffer layer, and formed of an oxide-based ceramic material comprising one selected from the group consisting of Ti, Zr, Al, Si, Ce, La, Sr, Cr, V, Nb, Ga, Ta, W, and Mo.

### Claim 2 (depends on 1)

The hydrogen separation membrane of claim 1, wherein the buffer layer is in the form of the plurality of columns having a diameter of 10 to 200nm.

### Claim 3 (depends on 2)

The hydrogen separation membrane of claim 2, wherein the plurality of columns of the buffer layer are formed separately, or formed in the form of a plurality of clusters.

### Claim 4 (depends on 1)

The hydrogen separation membrane of claim 1, wherein the buffer layer comprises:
a third buffer layer formed on the second buffer layer, and formed of one oxide-based ceramic material selected from the group consisting of TiOy, ZrOy, and Al2Oz where the composition of oxygen is 1<y<1.8, or 2<z<2.8.

### Claim 5

A method for manufacturing a hydrogen separation membrane, comprising:
preparing a porous support made of a metal or ceramic material;
forming a buffer layer in the form of a plurality of columns on the porous support, wherein the buffer layer is made of a ceramic material, and formed of a plurality of layers; and
forming a palladium-based metal separation membrane, which is able to separate hydrogen, on the buffer layer,
wherein the buffer layer has neighboring layers formed of different ceramic materials,
the forming of the buffer layer comprises:
forming a first buffer layer on the porous support wherein the first buffer layer is formed of one oxide-based ceramic material selected from the group consisting of TiOy, ZrOy, and Al2Oz where the composition of oxygen is 1<y<2, or 2<z<3;
forming a second buffer layer on the first buffer layer wherein the second buffer layer is formed of an oxide-based ceramic material comprising one selected from the group consisting of Ti, Zr, Al, Si, Ce, La, Sr, Cr, V, Nb, Ga, Ta, W, and Mo; and
forming a third buffer layer on the second buffer layer wherein the third buffer layer is formed of one oxide-based ceramic material selected from the group consisting of TiOy, ZrOy, and Al2Oz where the composition of oxygen is 1<y<2, or 2<z<3.

### Claim 6 (depends on 5)

The method of claim 5, wherein, in the forming of the buffer layer, the buffer layer is formed at a vacuum condition by means of a sputtering process using a target as MO2 (M is Ti or Zr) or Al2O3.

### Claim 7 (depends on 5)

The method of claim 5, wherein, in the forming of the buffer layer, the buffer layer is formed by supplying oxygen gas to an M metal plate or powder used as a source and oxidizing the M metal plate or powder by a reaction of evaporated M with the oxygen gas to grow on the porous support in the form of columns.

### Claim 8 (depends on 5)

The method of claim 5, wherein, in the forming of the metal separation membrane, the palladium-based metal separation membrane is formed on the buffer layer using a physical vapor deposition method.

### Claim 9

A hydrogen separation membrane comprising:
a porous support made of a metal or ceramic material;
a buffer layer made of a ceramic material, and formed in the form of a plurality of columns on the porous support, wherein the buffer layer is formed of a plurality of layers; and
a palladium-based metal separation membrane formed on the buffer layer and capable of separating hydrogen,
wherein the buffer layer has neighboring layers formed of different ceramic materials,
the buffer layer comprises:
a first buffer layer formed on the porous support, and formed of one oxide-based ceramic material selected from the group consisting of TiOy, ZrOy, and Al2Oz where the composition of oxygen is 1<y<2, or 2<z<3;
a second buffer layer formed on the first buffer layer, and formed of an oxide-based ceramic material comprising one selected from the group consisting of Ti, Zr, Al, Si, Ce, La, Sr, Cr, V, Nb, Ga, Ta, W, and Mo; and
a third buffer layer formed on the second buffer layer, and formed of one oxide-based ceramic material selected from the group consisting of TiOy, ZrOy, and Al2Oz where the composition of oxygen is 1<y<2, or 2<z<3.

### Claim 10 (depends on 9)

The hydrogen separation membrane of claim 9, wherein the buffer layer is in the form of the plurality of columns having a diameter of 10 to 200 nm.

### Claim 11 (depends on 9)

The hydrogen separation membrane of claim 9, wherein the plurality of columns of the buffer layer are formed separately, or formed in the form of a plurality of clusters.

### Claim 12 (depends on 9)

The hydrogen separation membrane of claim 9, wherein the composition of oxygen is 1.5<y <1.8, or 2<z<2.8.

### Claim 13 (depends on 1)

The hydrogen separation membrane of claim 1, wherein the composition of oxygen is 1.5<y <1.8, or 2<z<2.8.

### Claim 14 (depends on 5)

The method for manufacturing a hydrogen separation membrane of claim 5, wherein the composition of oxygen is 1.5<y<1.8, or 2<z<2.8.