# US 9,433,889 B2 · Palladium alloy membrane unit, storage structure thereof, and method of purifying hydrogen by using the same

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- Number: US 9,433,889 B2
- Document ID: US9433889B2
- Status: Granted
- Kind: B2
- Application number: 14/581,284
- Filed: 2014-12-23
- Published: 2015-07-16
- Granted: 2016-09-06
- Earliest claimed: 2014-01-16
- Assignees: Japan Pionics Co., Ltd.
- Applicants: Japan Pionics Co., Ltd.
- Inventors: Yoshinao Komiya; Satoshi Arakawa; Toshio Akiyama; Yasuo Sato; Noboru Takemasa
- Web page: https://patentgrep.com/patent/US9433889B2

## CPC

- B01D 53/228: {characterised by specific membranes}
- B01D 63/024: {with a single potted end}
- B01D 71/02231: {Palladium}
- C01B 3/505: Membranes containing palladium
- B01D 2053/223: {with hollow tubes}
- B01D 2256/16: Hydrogen
- B01D 2313/21: Specific headers, end caps
- C01B 2203/0233: the reforming step being a steam reforming step
- C01B 2203/0405: Purification by membrane separation
- C01B 2203/043: Regenerative adsorption process in two or more beds, one for adsorption, the other for regeneration
- C01B 2203/046: Purification by cryogenic separation
- 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}

## Abstract

The present invention is to provide a means for easily replacing palladium alloy capillaries in a hydrogen purification device formed by using hydrogen separation membrane formed from the palladium alloy capillaries. The hydrogen purification device can be easily disassembled into a palladium alloy membrane unit and a storage structure thereof. A palladium alloy membrane unit is provided with a plurality of palladium alloy capillaries, a disk-shaped tube sheet supporting the palladium alloy capillaries, a pure hydrogen discharge pipe having a cylinder being in close contact with a periphery of the tube sheet at one end, a joint connecting with a pure hydrogen outlet of the storage structure at the other end, and preferably a joint being in close contact with an opening of a container of the storage structure at a position between the cylinder and the outlet joint. The storage structure is provided with a container storing the palladium alloy membrane unit, a heater, a raw material hydrogen inlet, an impurity-containing gas outlet, and a pure hydrogen outlet, a member provided on the pure hydrogen outlet, the member connecting with a joint provided at one end of the palladium alloy membrane unit, and preferably a member provided on the opening of the container, the member being in close contact with a joint provided on the cylinder of the palladium alloy membrane unit.

## Claims

### Claim 1

A palladium alloy membrane unit stored in a container and integrated with a storage structure to make up a hydrogen purification device, the storage structure being provided with the container, a raw material hydrogen inlet, and a pure hydrogen outlet, comprising:
a plurality of palladium alloy capillaries; a tube sheet; and a pure hydrogen discharge pipe, wherein
the plurality of palladium alloy capillaries each have a closed end and an open end,
the closed end is formed by closing one end of each of the plurality of palladium alloy capillaries,
the open end is formed at the other end of each of the plurality of palladium alloy capillaries,
the tube sheet has a disk-shaped periphery and a plurality of supports,
the plurality of supports each support each of the plurality of palladium alloy capillaries at their respective open ends, and
the discharge pipe has an discharge pipe body, a cylinder formed at one end of the discharge pipe body, the cylinder being in close contact with the periphery, an outlet joint formed at the other end of the discharge pipe body and connected with the pure hydrogen outlet, and a container joint is in close contact with an opening of the container at a position between the cylinder and the outlet joint.

### Claim 2 (depends on 1)

The palladium alloy membrane unit according to claim 1, wherein the tube sheet, the discharge pipe, the outlet joint, and the container joint are coaxially set.

### Claim 3 (depends on 1)

The palladium alloy membrane unit according to claim 1, wherein
the outlet joint has a detaching part having a capability of attaching to and detaching from a connecting member provided in the storage structure for connecting with the outlet joint, and
the container joint has a detaching part having a capability of attaching to and detaching from a contact member provided in the storage structure for being in close contact with the container joint.

### Claim 4 (depends on 1)

A storage structure storing the palladium alloy membrane unit according to claim 1 and making up a hydrogen purification device together with the palladium alloy membrane unit, comprising:
a container having an opening formed at the end and a contact member in the opening, the contact member having a capability of being in close contact with the container joint, the container storing the plurality of palladium alloy capillaries inserted from the opening;
a heater heating the inside of the container from the outside;
a raw material hydrogen inlet supplying raw material hydrogen containing impurities to the container;
an impurity-containing gas outlet removing gas containing impurities not permeating the palladium alloy capillaries from the container; and
a pure hydrogen outlet having a connecting member having a capability of connecting with the outlet joint.

### Claim 5 (depends on 4)

A method of purifying hydrogen using the palladium alloy membrane unit stored in the storage structure according to claim 4, comprising:
after the plurality of palladium alloy capillaries are used for a predetermined period,
after the mechanical strength of the plurality of palladium alloy capillaries decreases, or
after gas leaks from around the plurality of palladium alloy capillaries,
replacing the palladium alloy membrane unit including the plurality of palladium alloy capillaries with a new one; and purifying hydrogen.
