# US 6,719,832 B2 · Hydrogen purification devices, components and fuel processing systems containing the same

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- Number: US 6,719,832 B2
- Document ID: US6719832B2
- Status: Granted
- Kind: B2
- Application number: 10/439,843
- Filed: 2003-05-15
- Published: 2003-11-06
- Granted: 2004-04-13
- Earliest claimed: 2001-09-27
- Assignees: IdaTech, LLC
- Inventors: David J. Edlund; Charles R. Hill; William A. Pledger; R. Todd Studebaker
- Web page: https://patentgrep.com/patent/US6719832B2

## CPC

- B01D 53/22: by diffusion (manufacturing semi-permeable membranes B01D67/00; form, structure or properties of semi-permeable membranes B01D69/00; material for semi-permeable membranes B01D71/00)
- B01D 63/06: Tubular membrane modules
- B01D 63/089: {Modules where the membrane is in the form of a bag, membrane cushion or pad}
- B01J 8/009: {Membranes, e.g. feeding or removing reactants or products to or from the catalyst bed through a membrane}
- C01B 3/38: using catalysts
- C01B 3/501: by diffusion
- C01B 3/503: characterised by membranes
- B01D 2313/221: Heat exchangers
- B01D 2313/42: Catalysts within the flow path
- B01D 2315/10: Cross-flow filtration
- B01J 2208/00539: Pressure
- B01J 2208/00548: Flow
- C01B 2203/0233: the reforming step being a steam reforming step
- C01B 2203/0405: Purification by membrane separation
- C01B 2203/041: In-situ membrane purification during hydrogen production
- C01B 2203/047: the impurity being carbon monoxide
- C01B 2203/0475: the impurity being carbon dioxide
- 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)
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}

## Abstract

A hydrogen purification device, components thereof, and fuel processors and fuel cell system containing the same. The hydrogen purification devices include an enclosure that contains a separation assembly adapted to receive a mixed gas stream containing hydrogen gas and to produce a stream that contains pure or at least substantially pure hydrogen gas therefrom. The separation assembly includes at least one hydrogen-permeable and/or hydrogen-selective membrane, and in some embodiments includes at least one membrane envelope that includes a pair of generally opposed membrane regions that define a harvesting conduit therebetween and which are separated by a support. The enclosure includes components that are formed from materials having similar or the same coefficients of thermal expansion as the membrane or membranes. In some embodiments, these components include at least a portion of the support, and in some embodiments, these components include at least a portion of the enclosure.

## Claims

### Claim 1

A fuel processing assembly, comprising:
a hydrogen-producing region adapted to produce a mixed gas stream containing hydrogen gas and other gases from a feed stream;
an enclosure defining an internal compartment; wherein the enclosure includes a pair of end plates and a shell portion that extends at least partially between the end plates to define at least a portion of the enclosure, wherein the enclosure is adapted to receive at least a portion of the mixed gas stream and to separate the mixed gas stream, via a pressure-driven separation process, into at least one product stream and at least one byproduct stream, and further wherein the enclosure further includes means for removing the at least one product stream from the internal compartment and means for removing the at least one byproduct stream from the internal compartment;
at least one hydrogen-selective membrane supported within the compartment, wherein the at least one hydrogen-selective membrane includes a first surface adapted to be contacted by the mixed gas stream and a permeate surface generally opposed to the first surface, wherein the product stream is formed from a portion of the mixed gas stream that passes through the at least one hydrogen-selective membrane to the permeate surface, and the byproduct stream is formed from a portion of the mixed gas stream that does not pass through the at least one hydrogen-selective membrane; and
a support structure adapted to support the at least one hydrogen-selective membrane within the compartment, wherein the support structure has a different composition than the at least one hydrogen-selective membrane, is formed from a composition that includes an alloy comprising nickel and copper, and has a coefficient of thermal expansion that is within approximately 10% of the coefficient of thermal expansion of the at least one hydrogen-selective membrane.

### Claim 2 (depends on 1)

The assembly of claim 1, wherein the support structure has a coefficient of thermal expansion that is within 5% of the coefficient of thermal expansion of the at least one hydrogen-selective membrane.

### Claim 3 (depends on 2)

The assembly of claim 2, wherein the support structure has a coefficient of thermal expansion that is within 2% of the coefficient of thermal expansion of the at least one hydrogen-selective membrane.

### Claim 4 (depends on 1)

The assembly of claim 1, wherein the support structure has a coefficient of thermal expansion that is less than the coefficient of thermal expansion of the at least one hydrogen-selective membrane.

### Claim 5 (depends on 4)

The assembly of claim 4, wherein the support structure has a coefficient of thermal expansion that is greater than approximately 13 μm/m/° C.

### Claim 6 (depends on 4)

The assembly of claim 4, wherein the support structure is metallic.

### Claim 7 (depends on 1)

The assembly of claim 1, wherein the at least one hydrogen-selective membrane is at least substantially formed from a palladium alloy that includes approximately 40 wt % copper.

### Claim 8 (depends on 1)

The assembly of claim 1, wherein the at least one hydrogen-selective membrane has a generally planar configuration.

### Claim 9 (depends on 1)

The assembly of claim 1, wherein the support structure is not hydrogen-selective.

### Claim 10 (depends on 1)

The assembly of claim 1, wherein the support structure includes at least one screen member.

### Claim 11 (depends on 1)

The assembly of claim 1, wherein the support structure includes a plurality of screen members.

### Claim 12 (depends on 11)

The assembly of claim 11, wherein the plurality of screen members includes at least one screen member that forms at least a portion of the support structure, and further wherein the plurality of screen members includes at least one screen member that does not contact the at least one hydrogen-selective membrane.

### Claim 13 (depends on 1)

The assembly of claim 1, wherein the enclosure is at least substantially formed from an alloy of nickel and copper.

### Claim 14 (depends on 1)

The assembly of claim 1, wherein the enclosure has a coefficient of thermal expansion that is less than 16 μm/m/° C.

### Claim 15 (depends on 1)

The assembly of claim 1, wherein the enclosure has a coefficient of thermal expansion that is less than the coefficient of thermal expansion of the at least one hydrogen-selective membrane.

### Claim 16 (depends on 1)

The assembly of claim 1, wherein each of the end plates includes a perimeter region, and further wherein at least a portion of the shell portion is integrally formed with a first one of the end plates and projects from the perimeter region thereof generally toward a second one of the end plates.

### Claim 17 (depends on 16)

The assembly of claim 16, wherein the shell portion includes an end portion distal the first one of the end plates that is adapted to form an at least substantially fluid-tight interface with a sealing region of the second one of the end plates.

### Claim 18 (depends on 16)

The assembly of claim 16, wherein the shell portion is a first shell portion that is integrally formed with the first one of the pair of end plates, wherein the enclosure further includes a second shell portion that is integrally formed with the second one of the end plates and which extends generally toward the first one of the end plates.

### Claim 19 (depends on 18)

The assembly of claim 18, wherein the shell portions include end regions that are adapted to collectively form an at least substantially fluid-tight interface.

### Claim 20 (depends on 19)

The assembly of claim 19, wherein the assembly further includes at least one seal member extending between the end regions.

### Claim 21 (depends on 16)

The assembly of claim 16, wherein the enclosure includes only a single interface between the pair of end plates and the shell portion.

### Claim 22 (depends on 16)

The assembly of claim 16, wherein the at least one hydrogen-selective membrane includes a pair of hydrogen-selective membranes that are oriented such that the pair of hydrogen-selective membranes are spaced-apart from each other with their permeate surfaces generally facing each other to define a membrane envelope with a harvesting conduit extending between the permeate surfaces, and further wherein the product stream is formed from the portion of the mixed gas stream that passes through the membranes to the harvesting conduit, with the remaining portion of the mixed gas stream which remains on the first surface of the membranes forming at least a portion of the byproduct stream.

### Claim 23 (depends on 22)

The assembly of claim 22, wherein the support structure extends within the harvesting conduit.

### Claim 24 (depends on 23)

The assembly of claim 23, further comprising a plurality of membrane envelopes.

### Claim 25 (depends on 23)

The assembly of claim 23, wherein the pair of hydrogen-selective membranes comprise an alloy of palladium and approximately 40 wt % copper.

### Claim 26 (depends on 1)

The assembly of claim 1, in combination with a fuel cell stack adapted to receive at least a portion of the product stream.

### Claim 27 (depends on 26)

The assembly of claim 26, in combination with at least one assembly adapted to reduce the concentration of any carbon monoxide present in the product stream.

### Claim 28 (depends on 1)

The assembly of claim 1, wherein the hydrogen-producing region includes a catalyst adapted to produce the mixed gas stream via steam reforming of a feed stream that includes water and at least one carbon-containing feedstock.

### Claim 29 (depends on 28)

The assembly of claim 28, in combination with a fuel cell stack adapted to receive at least a portion of the product stream.

### Claim 30 (depends on 29)

The assembly of claim 29, in combination with at least one assembly adapted to reduce the concentration of any carbon monoxide present in the product stream.

### Claim 31

A hydrogen purification device, comprising
an enclosure defining an internal compartment; wherein the enclosure is adapted to receive a mixed gas stream comprising hydrogen gas and other gases and having a temperature of at least 300° C. and a pressure of at least 100 psi, wherein the enclosure includes means for receiving the mixed gas stream into the internal compartment, means for removing a byproduct stream from the internal compartment and means for removing a product hydrogen stream from the internal compartment;
at least one hydrogen-selective membrane supported within the compartment, wherein the at least one hydrogen-selective membrane is formed from an alloy of palladium and copper and has a coefficient of thermal expansion, wherein the at least one hydrogen-selective membrane includes a first surface adapted to be contacted by the mixed gas stream and a permeate surface generally opposed to the first surface, and further wherein the product hydrogen stream is formed from a portion of the mixed gas stream that passes through the at least one hydrogen-selective membrane to the permeate surface, and the byproduct stream is formed from a portion of the mixed gas stream that does not pass through the at least one hydrogen-selective membrane; and
a membrane-contacting structure that is in contact with at least one of the first or the permeate surfaces of the membrane, wherein the membrane-contacting structure is selected to have a coefficient of thermal expansion that is sufficiently close to or equal to the coefficient of thermal expansion of the at least one hydrogen-selective membrane such that upon thermal cycling of the device within a temperature range of at least 200° C. the membrane-contacting structure is adapted to not impart wrinkle-inducing forces to the at least one hydrogen-selective membrane.

### Claim 32 (depends on 31)

The device of claim 31, wherein the membrane-contacting structure includes an alloy comprising nickel and copper.

### Claim 33 (depends on 31)

The device of claim 31, wherein the membrane-contacting structure has a coefficient of thermal expansion that is the same as or less than the coefficient of thermal expansion of the at least one hydrogen-selective membrane.

### Claim 34 (depends on 31)

The device of claim 31, wherein the enclosure is formed from one or more materials selected such that upon thermal cycling of the device within the temperature range the enclosure does not impart wrinkle-inducing forces to the at least one hydrogen-selective membrane.

### Claim 35 (depends on 34)

The device of claim 34, wherein the enclosure includes an alloy comprising nickel and copper.

### Claim 36 (depends on 35)

The device of claim 35, wherein the enclosure has a coefficient of thermal expansion that is the same as or less than the coefficient of thermal expansion of the at least one membrane.

### Claim 37 (depends on 31)

The device of claim 31, wherein the at least one hydrogen-selective membrane is formed from an alloy of palladium and approximately 40 wt % copper.

### Claim 38 (depends on 31)

The device of claim 31, in combination with a fuel processing assembly that is adapted to receive a feed stream and to produce the mixed gas stream therefrom.

### Claim 39 (depends on 38)

The device of claim 38, wherein the fuel processing assembly includes at least one reforming catalyst bed and further wherein the feed stream contains water and a carbon-containing feedstock.

### Claim 40 (depends on 39)

The device of claim 39, wherein the at least one reforming catalyst bed and the enclosure are at least partially housed within a common shell.

### Claim 41 (depends on 38)

The device of claim 38, in further combination with a fuel cell stack adapted to receive at least a portion of the product hydrogen stream and to produce an electric current therefrom.

### Claim 42 (depends on 41)

The device of claim 41, further comprising an assembly adapted to reduce the concentration of any carbon monoxide present in the product hydrogen stream.

### Claim 43 (depends on 31)

The device of claim 31, in further combination with a fuel cell stack adapted to receive at least a portion of the product hydrogen stream and to produce an electric current therefrom.

### Claim 44 (depends on 43)

The device of claim 43, further comprising an assembly adapted to reduce the concentration of any carbon monoxide present in the product hydrogen stream.
