Edlund, David J. (Bend, OR, US)
Pledger, William A. (Bend, OR, US)
Studebaker, Todd R. (Bend, OR, US)

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422/211, 48/61, 48/DIG.5, 48/127.9, 422/193, 96/7, 429/19, 423/652, 422/198, 48/76, 96/11

B01D53/22; B01J8/02; C01B3/26

96/4, 48/61, 422/211, 48/DIG.5, 95/56, 48/76, 95/45, 423/651, 48/127.9, 422/187, 422/193, 429/19, 48/156.5, 429/12, 429/20, 422/189, 95/55, 96/8, 96/7, 422/188, 423/650, 429/17, 96/10, 48/127.7, 48/63, 422/198, 423/652, 96/11

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3368329	Hydrogen purification apparatus	February, 1968	Eguchi et al.
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3447288	GAS-DIFFUSION ASSEMBLY INCLUDING THIN HYDROGEN-PERMEABLE IMPERVIOUS FOIL	June, 1969	Juda et al.
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3486301	HYDROGEN DIFFUSION APPARATUS	December, 1969	Bonnet
3520803	MEMBRANE FLUID SEPARATION APPARATUS AND PROCESS	July, 1970	Iaconelli
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3524819	STEAM REFORMING OF HYDROCARBONS	August, 1970	Guerrieri
3534531	ASSEMBLY OF PURE GAS PERMEATING SEPARATOR	October, 1970	Eguchi et al.
3564819		February, 1971	Neukander et al.
3589171	GAS ANALYSIS SYSTEM AND PALLADIUM TUBE SEPARATOR THEREFOR	June, 1971	Haley
3665680	HYDROGEN DIFFUSION APPARATUS	May, 1972	Heuser
3713270	HYDROGEN DIFFUSION MEMBRANES	January, 1973	Farr et al.
3761382		September, 1973	Hammond et al.
3782904		January, 1974	Fletcher
3787038	REFORMER FOR FIRING REVERBERATORY FURNACE AND METHOD OF OPERATING SAID REFORMER	January, 1974	Tesner et al.
3791106	GAS ANALYSIS SYSTEMS AND PALLADIUM TUBE SEPARATOR THEREFOR	February, 1974	Haley
3839110	CHEMICAL ETCHANT FOR PALLADIUM	October, 1974	Shankoff
3849076	CATALYTIC REACTOR FOR CARRYING OUT CONJUGATE CHEMICAL REACTIONS	November, 1974	Gryaznov et al.
3881891	Method for preparation of super-high purity hydrogen	May, 1975	Goltsov et al.
3881897	Apparatus for separating fluids	May, 1975	Faure et al.
3920416	Hydrogen-rich gas generator	November, 1975	Houseman
3955941	Hydrogen rich gas generator	May, 1976	Houseman et al.
3972695	Hydrogen purifier	August, 1976	Buckley et al.
3980452	Process for supplying heat to chemical reactions	September, 1976	Krumm et al.
3982910	Hydrogen-rich gas generator	September, 1976	Houseman et al.
4003343	Method and apparatus for maintaining the operating temperature in a device for reducing engine exhaust pollutants	January, 1977	Lee
4003725	Apparatus for purifying hydrogen gas	January, 1977	Bunn, Jr. et al.
4056373	Hydrogen-purification apparatus with palladium-alloy filter coil	November, 1977	Rubin
4078985	Hydrogen generator	March, 1978	Takeuchi
4084934	Combustion apparatus	April, 1978	Kumazawa
4098959	Fuel cell fuel control system	July, 1978	Fanciullo
4098960	Fuel cell fuel control system	July, 1978	Gagnon
4127393	Method and apparatus for vaporizing hydrocarbon based liquids	November, 1978	Timmins et al.
4132668	Method of preparing a hydrogen-permeable membrane catalyst on a base of palladium or its alloys for the hydrogenation of unsaturated organic compounds	January, 1979	Gryaznov et al.
4134739	Starting device for a reformed gas generator	January, 1979	Gulden et al.
4197152	Attaching self-supporting emissive film to cathode support	April, 1980	Palty et al.
4238403	Methanol synthesis process	December, 1980	Pinto
4248688	Ion milling of thin metal films	February, 1981	Gartner et al.
4254086	Endothermal water decomposition unit for producing hydrogen and oxygen	March, 1981	Sanders
4302177	Fuel conversion apparatus and method	November, 1981	Fankhanel et al.
4313013	Palladium or a palladium alloy hydrogen diffusion membrane treated with a volatile compound of silicon is used to separate hydrogen from a mixture of it with a hydrocarbon	January, 1982	Harris
4315893	Reformer employing finned heat pipes	February, 1982	McCallister
4319923	Recovery of gold and/or palladium from an iodide-iodine etching solution	March, 1982	Falanga et al.
4329157	Inorganic anisotropic hollow fibers	May, 1982	Dobo et al.
4331520	Process for the recovery of hydrogen-reduced metals, ions and the like at porous hydrophobic catalytic barriers	May, 1982	Juda et al.
4349613	Method and apparatus for electrochemical energy production	September, 1982	Winsel
4381641	Substoichiometric combustion of low heating value gases	May, 1983	Madgavkar et al.
4387434	Intelligent field interface device for fluid storage facility	June, 1983	Moncrief, Jr. et al.
4400182	Vaporization and gasification of hydrocarbon feedstocks	August, 1983	Davies et al.
4417905	Gas making	November, 1983	Banks et al.
4422911	Method of recovering hydrogen-reduced metals, ions and the like at porous catalytic barriers and apparatus therefor	December, 1983	Juda et al.
4430304	Slab reformer	February, 1984	Spurrier et al.
4444158	Alcohol dissociation process for automobiles	April, 1984	Yoon
4468235	Hydrogen separation using coated titanium alloys	August, 1984	Hill
4472176	Apparatus and method for the production of pure hydrogen from a hydrogen-containing crude gas	September, 1984	Rubin
4473622	Rapid starting methanol reactor system	September, 1984	Chludzinski et al.
4504447	Slab reformer	March, 1985	Spurrier et al.
4533607	Process for removing electrolyte vapor from fuel cell exhaust gas	August, 1985	Sederquist
4553981	Enhanced hydrogen recovery from effluent gas streams	November, 1985	Fuderer
4567857	Combustion engine system	February, 1986	Houseman et al.
4589891	Hydrogen permeatin membrane, process for its manufacture and use	May, 1986	Iniotakis et al.
4642273	Reformer reaction control apparatus for a fuel cell	February, 1987	Sasaki
4644751	Integrated fuel-cell/steam plant for electrical generation	February, 1987	Hsu
4650814	Process for producing methanol from a feed gas	March, 1987	Keller
4654063	Process for recovering hydrogen from a multi-component gas stream	March, 1987	Auvil et al.
4655797	Fine screen and fine screen stack, their use and process for the manufacture of fine screens	April, 1987	Iniotakis et al.
4657828	Fuel cell system	April, 1987	Tajima
4659634	Methanol hydrogen fuel cell system	April, 1987	Struthers
4670359	Fuel cell integrated with steam reformer	June, 1987	Beshty et al.
4684581	Hydrogen diffusion fuel cell	August, 1987	Struthers
4699637	Hydrogen permeation membrane	October, 1987	Iniotakis et al.
4707267	Device and method for separating individual fluids from a mixture of fluids	November, 1987	Johnson	96/8
4713234	Process and apparatus for conversion of water vapor with coal or hydrocarbon into a product gas	December, 1987	Weirich et al.
4751151	Recovery of carbon dioxide from fuel cell exhaust	June, 1988	Healy et al.
4781241	Heat exchanger for fuel cell power plant reformer	November, 1988	Misage et al.
4788004	Catalytic process	November, 1988	Pinto et al.
4810485	Hydrogen forming reaction process	March, 1989	Marianowski et al.
4838897	Reformer	June, 1989	Amano et al.
4849187	Steam reforming apparatus	July, 1989	Uozu et al.
4865624	Method for steam reforming methanol and a system therefor	September, 1989	Okada
4880040	Liquid petroleum confinement system	November, 1989	Pierson et al.
4904455	Production of synthesis gas using convective reforming	February, 1990	Karafian et al.
4904548	Method for controlling a fuel cell	February, 1990	Tajima
4946667	Method of steam reforming methanol to hydrogen	August, 1990	Beshty
4981676	Catalytic ceramic membrane steam/hydrocarbon reformer	January, 1991	Minet et al.
4999107	Separator frame for a two-fluid exchanger device	March, 1991	Guerif
5030661	Hydrogen production	July, 1991	Lywood
5032365	Reaction apparatus	July, 1991	Aono et al.
5126045	Support plates with meandrical channels for diaphragm filtration	June, 1992	Kohlheb et al.
5139541	Hydrogen-permeable composite metal membrane	August, 1992	Edlund
5158581	Fluid separation membrane module with hollow fibers having segregated active surface regions	October, 1992	Coplan
5205841	Apparatus and method for extracting hydrogen	April, 1993	Vaiman
5215729	Composite metal membrane for hydrogen extraction	June, 1993	Buxbaum
5217506	Hydrogen-permeable composite metal membrane and uses thereof	June, 1993	Edlund et al.
5225080	Filtration module and device for separating and filtering fluids in a crossflow process	July, 1993	Karbachsch et al.
5226928	Reforming apparatus for hydrocarbon	July, 1993	Makabe et al.
5229102	Catalytic ceramic membrane steam-hydrocarbon reformer	July, 1993	Minet et al.
5259870	Hydrogen-permeable composite metal membrane	November, 1993	Edlund
5326550	Fluidized bed reaction system for steam/hydrocarbon gas reforming to produce hydrogen	July, 1994	Adris et al.
5335628	Integrated boiler/fuel cell system	August, 1994	Dunbar
5344721	Solid polymer electrolyte fuel cell apparatus	September, 1994	Sonai et al.
5354547	Hydrogen recovery by adsorbent membranes	October, 1994	Rao et al.
5376167	Purifying device for hydrogen comprising a base made of an alloy of the same composition as that of the tubes	December, 1994	Broutin et al.
5382271	Hydrogen generator	January, 1995	Ng et al.
5393325	Composite hydrogen separation metal membrane	February, 1995	Edlund
5395425	Apparatus employing porous diaphragms for producing useful work	March, 1995	Brown
5401589	Application of fuel cells to power generation systems	March, 1995	Palmer et al.
5417051	Process and installation for the combined generation of electrical and mechanical energy	May, 1995	Ankersmit et al.
RE35002	Fuel cell system	July, 1995	Matsubara et al.
5432710	Energy supply system for optimizing energy cost, energy consumption and emission of pollutants	July, 1995	Ishimaru et al.
5449848	Dehydrogenation process	September, 1995	Itoh
5458857	Combined reformer and shift reactor	October, 1995	Collins et al.
5498278	Composite hydrogen separation element and module	March, 1996	Edlund
5500122	Stacked fluid-separation membrane disk module assemblies	March, 1996	Schwartz
5509942	Manufacture of tubular fuel cells with structural current collectors	April, 1996	Dodge
5516344	Fuel cell power plant fuel processing apparatus	May, 1996	Corrigan
5518530	Connected body comprising a gas separator and a metal, and apparatus for separating hydrogen gas from a mixed gas	May, 1996	Sakai et al.
5520807	Stacked fluid-separation membrane disk module assemblies	May, 1996	Myrna et al.
5525322	Method for simultaneous recovery of hydrogen from water and from hydrocarbons	June, 1996	Willms
5527632	Hydrocarbon fuelled fuel cell power system	June, 1996	Gardner
5536405	Stacked membrane disk assemblies for fluid separations	July, 1996	Myrna et al.
5580523	Integrated chemical synthesizers	December, 1996	Bard
5589599	Pyrolytic conversion of organic feedstock and waste	December, 1996	McMullen et al.
5612012	Method for removing carbon monoxide from reformed gas	March, 1997	Soma et al.
5616430	Reformer and fuel cell system using the same	April, 1997	Aoyama
5637259	Process for producing syngas and hydrogen from natural gas using a membrane reactor	June, 1997	Galuszka et al.
5637414	Method and system for controlling output of fuel cell power generator	June, 1997	Inoue et al.
5639431	Hydrogen producing apparatus	June, 1997	Shirasaki et al.
5645626	Composite hydrogen separation element and module	July, 1997	Edlund et al.
5658681	Fuel cell power generation system	August, 1997	Sato et al.
5677073	Fuel cell generator and method of the same	October, 1997	Kawatsu
5679249	Dynamic filter system	October, 1997	Fendya et al.
5705082	Roughening of metal surfaces	January, 1998	Hinson
5705916	Process for the generation of electrical power	January, 1998	Rudbeck et al.
5712052	Fuel cell generator and method of the same	January, 1998	Kawatsu
5714276	Method for supplying fuel gas to fuel cell assembly	February, 1998	Okamoto
5734092	Planar palladium structure	March, 1998	Wang et al.
5738708	Composite metal membrane	April, 1998	Peachey et al.
5741474	Process for production of high-purity hydrogen	April, 1998	Isomura et al.
5741605	Solid oxide fuel cell generator with removable modular fuel cell stack configurations	April, 1998	Gillett et al.
5780179	Fuel cell system for use on mobile bodies	July, 1998	Okamoto
5782960	Hydrogen separation member	July, 1998	Ogawa et al.
5795666	Modular power station for the production primarily of hydrogen from solar energy and a method of generating electric energy	August, 1998	Johnssen
5811065	Burner exhaust gas collection assembly for a catalytic reformer	September, 1998	Sterenberg
5814112	Nickel/ruthenium catalyst and method for aqueous phase reactions	September, 1998	Elliot et al.
5821185	Solid state proton and electron mediating membrane and use in catalytic membrane reactors	October, 1998	White et al.
5833723	Hydrogen generating apparatus	November, 1998	Kuwabara et al.
5858314	Thermally enhanced compact reformer	January, 1999	Hsu et al.
5861137	Steam reformer with internal hydrogen purification	January, 1999	Edlund
5874051	Method and apparatus for selective catalytic oxidation of carbon monoxide	February, 1999	Heil et al.
5888273	High temperature gas purification system	March, 1999	Buxbaum
5897766	Apparatus for detecting carbon monoxide, organic compound, and lower alcohol	April, 1999	Kawatsu
5897970	System for production of high-purity hydrogen, process for production of high-purity hydrogen, and fuel cell system	April, 1999	Isomura et al.
5904754	Diffusion-bonded palladium-copper alloy framed membrane for pure hydrogen generators and the like and method of preparing the same	May, 1999	Juda et al.
5931987	Apparatus and methods for gas extraction	August, 1999	Buxbaum
5932181	Natural gas-using hydrogen generator	August, 1999	Kim et al.
5938800	Compact multi-fuel steam reformer	August, 1999	Verrill et al.
5985474	Integrated full processor, furnace, and fuel cell system for providing heat and electrical power to a building	November, 1999	Chen et al.
5997594	Steam reformer with internal hydrogen purification	December, 1999	Edlund et al.
5998053	Method for operating an apparatus with fuel cells	December, 1999	Diethelm
6007931	Mass and heat recovery system for a fuel cell power plant	December, 1999	Fuller et al.
6042956	Method for the simultaneous generation of electrical energy and heat for heating purposes	March, 2000	Lenel
6045772	Method and apparatus for injecting a liquid hydrocarbon fuel into a fuel cell power plant reformer	April, 2000	Szydlowski et al.
6045933	Method of supplying fuel gas to a fuel cell	April, 2000	Okamoto
6054229	System for electric generation, heating, cooling, and ventilation	April, 2000	Hsu et al.
6077620	Fuel cell system with combustor-heated reformer	June, 2000	Pettit
6083637	Fuel cell energy generating system	July, 2000	Walz et al.
6103028	Method of fabricating thinned free-standing metallic hydrogen-selective palladium-bearing membranes and novel pin-hole-free membranes formed thereby	August, 2000	Juda et al.
6103411	Hydrogen production apparatus and method operable without supply of steam and suitable for fuel cell systems	August, 2000	Matsubayashi et al.
6152995	Hydrogen-permeable metal membrane and method for producing the same	November, 2000	Edlund
6165633	Method of and apparatus for reforming fuel and fuel cell system with fuel-reforming apparatus incorporated therein	December, 2000	Negishi
6168650	High temperature gas purification apparatus	January, 2001	Buxbaum
6171574	Method of linking membrane purification of hydrogen to its generation by steam reforming of a methanol-like fuel	January, 2001	Juda et al.
6183543	Apparatus and methods for gas extraction	February, 2001	Buxbuam
6190623	Apparatus for providing a pure hydrogen stream for use with fuel cells	February, 2001	Sanger et al.
6201029	Staged combustion of a low heating value fuel gas for driving a gas turbine	March, 2001	Waycuilis
6221117	Hydrogen producing fuel processing system	April, 2001	Edlund et al.	48/76
6238465	Method of producing thin palladium-copper and the like, palladium alloy membranes by solid-solid metallic interdiffusion, and improved membrane	May, 2001	Juda et al.
6242120	System and method for optimizing fuel cell purge cycles	June, 2001	Herron
6319306	Hydrogen-selective metal membrane modules and method of forming the same	November, 2001	Edlund et al.
6395405	Hydrogen permeable membrane and hydride battery composition	May, 2002	Buxbaum
6458189	Hydrogen-selective metal membrane modules and method of forming the same	October, 2002	Edlund et al.	96/7
6461408	Hydrogen generator	October, 2002	Buxbaum
6494937	Hydrogen purification devices, components and fuel processing systems containing the same	December, 2002	Edlund et al.
6537352	Hydrogen purification membranes, components and fuel processing systems containing the same	March, 2003	Edlund et al.
6547858	Hydrogen-permeable metal membrane and hydrogen purification assemblies containing the same	April, 2003	Edlund et al.
6562111	Hydrogen purification devices, components and fuel processing systems containing the same	May, 2003	Edlund et al.	96/4
6632270	Hydrogen purification membranes, components and fuel processing systems containing the same	October, 2003	Edlund et al.
6719832	Hydrogen purification devices, components and fuel processing systems containing the same	April, 2004	Edlund et al.	96/4
6767389	Hydrogen-selective metal membranes, membrane modules, purification assemblies and methods of forming the same	July, 2004	Edlund et al.	96/11

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Greene, Jason M.

Dascenzo Intellectual Property Law, P.C.

RELATED APPLICATIONS

This application is a continuation of and claims priority to U.S. patent application Ser. No. 11/441,931, which was filed on May 25, 2006, issued on Mar. 27, 2007 as U.S. Pat. No. 7,195,663, and which is a continuation of U.S. patent application Ser. No. 10/989,907, which was filed on Nov. 15, 2004, issued on May 30, 2006 as U.S. Pat. No. 7,052,530, and which is a continuation of U.S. patent application Ser. No. 10/728,473, now U.S. Pat. No. 6,824,593, which was filed on Dec. 5, 2003, and which is a continuation of U.S. patent application Ser. No. 10/430,110, now U.S. Pat. No. 6,723,156, which was filed on May 5, 2003, and which is a continuation of U.S. patent application Ser. No. 10/371,597, now U.S. Pat. No. 6,632,270, which was filed on Feb. 20, 2003, and which is a continuation of U.S. patent application Ser. No. 10/027,509, now U.S. Pat. No. 6,537,352, which was filed on Dec. 19, 2001. U.S. patent application Ser. No. 10/027,509 is a continuation-in-part of and claims priority to U.S. patent application Ser. Nos. 09/839,997, 09/618,866, and 09/967,172. U.S. patent application Ser. No. 09/839,997, was filed on Apr. 20, 2001 now U.S. Pat. No. 6,783,741 and is a continuation of U.S. patent application Ser. No. 09/291,447, now U.S. Pat. No. 6,221,117, which was filed on Apr. 13, 1999 and which is a continuation-in-part application of U.S. patent application Ser. No. 08/951,091, now U.S. Pat. No. 5,997,594, which was filed on Oct. 15, 1997, and which is a continuation-in-part application of U.S. patent application Ser. No. 08/741,057, now U.S. Pat. No. 5,861,137, which was filed on Oct. 30, 1996. U.S. patent application Ser. No. 09/618,866, now U.S. Pat. No. 6,547,858, was filed on Jul. 19, 2000 and is a continuation-in-part application of U.S. patent application Ser. No. 09/274,154, now U.S. Pat. No. 6,152,995, which was filed on Mar. 22, 1999. U.S. patent application Ser. No. 09/967,172, now U.S. Pat. No. 6,494,937, was filed on Sep. 27, 2001. The complete disclosures of the above-identified patent applications are hereby incorporated by reference for all purposes.

We claim:

1. A hydrogen-producing fuel processing assembly, comprising: a hydrogen-producing region adapted to produce a mixed gas stream from at least one feed stream, wherein the mixed gas stream includes hydrogen gas as a majority component and other gases; an enclosure defining an internal compartment having an internal surface; a separation assembly within the internal compartment, wherein the separation assembly is adapted to receive a mixed gas stream and to divide the mixed gas stream into a hydrogen-rich permeate stream, which has a greater concentration of hydrogen gas than the mixed gas stream, and a byproduct stream, which comprises a greater concentration of the other gases than the mixed gas stream, and further wherein the separation assembly comprises: at least one hydrogen-selective membrane having a mixed gas surface and a permeate surface, wherein the permeate stream includes hydrogen gas that permeates through the membrane from the mixed gas surface to the permeate surface, and further wherein the byproduct stream includes at least a portion of the mixed gas stream that does not permeate through the membrane; a support structure for the at least one hydrogen-selective membrane; and at least one guide structure projecting from the enclosure into the internal compartment to define a position for the separation assembly within the internal compartment.

2. The assembly of claim 1, wherein the device includes a plurality of guide structures that project into the internal compartment to define the position of the separation assembly within the internal compartment.

3. The assembly of claim 1, wherein the guide structure includes a rib that projects into the internal compartment.

4. The assembly of claim 1, wherein the enclosure is formed from a material, and further wherein the guide structure is formed from the same material as the enclosure.

5. The assembly of claim 4, wherein the guide structure is integrally formed with the enclosure.

6. The assembly of claim 1, wherein the separation assembly includes a plurality of hydrogen-selective membranes.

7. The assembly of claim 1, wherein the separation assembly includes at least a plurality of hydrogen-selective membranes, each having a mixed gas surface and a permeate surface, wherein the hydrogen-selective membranes are spaced-apart from each other and oriented with their permeate surfaces generally facing each other to define a harvesting conduit extending therebetween, and further wherein the permeate stream is formed from at least a portion of the mixed gas stream that passes through the hydrogen-selective membranes to the harvesting conduit, with the byproduct stream being formed from at least a portion of the mixed gas stream that remains on the mixed gas surface of the hydrogen-selective membranes, wherein the separation assembly further includes a support within the harvesting conduit and adapted to support the plurality of hydrogen-selective membranes, and further wherein the support includes a pair of generally opposed surfaces which are adapted to provide support to a respective one of the permeate surfaces of the hydrogen-selective membranes.

8. The assembly of claim 7, wherein the support is adapted to permit flow of gas both parallel and transverse to the permeate surfaces of the membranes.

9. The assembly of claim 1, wherein the enclosure includes an input port adapted to receive the mixed gas stream from the hydrogen-producing region.

10. The assembly of claim 1, wherein the hydrogen-producing region is located within the internal compartment, and further wherein the enclosure includes an input port adapted to receive the at least one feed stream.

11. The assembly of claim 1, further comprising a vaporization region adapted to receive and vaporize a liquid feed stream comprising a carbon-containing feedstock and water.

12. The assembly of claim 1, further comprising a polishing catalyst bed including a methanation catalyst, wherein the polishing catalyst bed is in fluid communication with the separation assembly and is adapted to receive the hydrogen-rich permeate stream therefrom and produce a product stream from the hydrogen-rich permeate stream, wherein the polishing catalyst bed is adapted to reduce the concentration of carbon dioxide and carbon monoxide in the hydrogen-rich permeate stream by catalytic reaction to produce methane.

13. The assembly of claim 12, wherein the polishing catalyst bed is at least partially located within the internal compartment of the enclosure.

14. The assembly of claim 13, wherein a portion of the polishing catalyst bed extends external the internal compartment of the enclosure.

15. The assembly of claim 12, wherein the polishing catalyst bed is located external the internal compartment of the enclosure.

16. The assembly of claim 1, wherein the separation assembly is adapted to produce a byproduct stream containing approximately 20-50% of the stoichiometrically available hydrogen gas in the mixed gas stream.

17. The assembly of claim 1, wherein the amount of hydrogen gas in the hydrogen-rich permeate stream is less than a stoichiometrically available amount of hydrogen gas.

18. The assembly of claim 1, wherein the amount of hydrogen gas in the hydrogen-rich permeate stream is between approximately 50% and approximately 80% of the stoichiometrically available hydrogen gas in the mixed gas stream.

19. The assembly of claim 1, further comprising a heating assembly that includes a combustion region adapted to receive and combust a fuel stream to produce a heated exhaust stream to heat the hydrogen-producing region.

20. The assembly of claim 1, wherein the fuel stream is at least partially comprised of the byproduct stream, and further wherein the byproduct stream contains at least 20 wt % hydrogen gas.

21. The assembly of claim 1, in combination with a fuel cell stack adapted to receive at least a portion of the hydrogen-rich permeate stream and to produce an electric current therefrom.

22. The assembly of claim 21, wherein the combustion region is adapted to receive air for supporting combustion from the fuel cell stack.

FIELD OF THE DISCLOSURE

The present invention is related generally to the purification of hydrogen gas, and more specifically to hydrogen purification membranes, devices, and fuel processing and fuel cell systems containing the same.

BACKGROUND OF THE DISCLOSURE

Purified hydrogen is used in the manufacture of many products including metals, edible fats and oils, and semiconductors and microelectronics. Purified hydrogen is also an important fuel source for many energy conversion devices. For example, fuel cells use purified hydrogen and an oxidant to produce an electrical potential. Various processes and devices may be used to produce the hydrogen gas that is consumed by the fuel cells. However, many hydrogen-production processes produce an impure hydrogen stream, which may also be referred to as a mixed gas stream that contains hydrogen gas. Prior to delivering this stream to a fuel cell, a stack of fuel cells, or another hydrogen-consuming device, the mixed gas stream may be purified, such as to remove undesirable impurities.

BRIEF DESCRIPTION OF THE DRAWINGS

FIG. 1 is a schematic view of a hydrogen purification device.

FIG. 2 is an isometric view of a hydrogen-permeable metal membrane.

FIG. 3 is a cross-sectional detail of the membrane of FIG. 2 with an attached frame.

FIG. 4 is an isometric view of the membrane of FIG. 2 after being etched according to a method of the present invention.

FIG. 5 is a cross-sectional detail of the membrane of FIG. 4.

FIG. 6 is an isometric view of the membrane of FIG. 2 with an absorbent medium placed over an application region of one of the membrane's surfaces.

FIG. 7 is a cross-sectional detail of the membrane of FIG. 6.

FIG. 8 is the detail of FIG. 4 with a hole indicated generally at 41 and the repaired hole indicated in dashed lines at 43 .

FIG. 9 is a schematic cross-sectional view of a hydrogen purification device having a planar separation membrane.

FIG. 10 is an isometric view of an illustrative end plate for a hydrogen purification device according to the present invention.

FIG. 11 is a schematic cross-sectional view of a hydrogen purification device having a tubular separation membrane.

FIG. 12 is a schematic cross-sectional view of another hydrogen purification device having a tubular separation membrane.

FIG. 13 is a schematic cross-sectional view of another enclosure for a hydrogen purification device constructed according to the present invention.

FIG. 14 is a schematic cross-sectional view of another enclosure for a hydrogen purification device constructed according to the present invention.

FIG. 15 is a fragmentary cross-sectional detail showing another suitable interface between components of an enclosure for a purification device according to the present invention.

FIG. 16 is a fragmentary cross-sectional detail showing another suitable interface between components of an enclosure for a purification device according to the present invention.

FIG. 17 is a fragmentary cross-sectional detail showing another suitable interface between components of an enclosure for a purification device according to the present invention.

FIG. 18 is a fragmentary cross-sectional detail showing another suitable interface between components of an enclosure for a purification device according to the present invention.

FIG. 19 is a top plan view of an end plate for a hydrogen purification device constructed according to the present invention.

FIG. 20 is a cross-sectional view of the end plate of FIG. 19.

FIG. 21 is a top plan view of an end plate for a hydrogen purification device constructed according to the present invention.

FIG. 22 is a cross-sectional view of the end plate of FIG. 21.

FIG. 23 is a top plan view of an end plate for a hydrogen purification device constructed according to the present invention.

FIG. 24 is a cross-sectional view of the end plate of FIG. 23.

FIG. 25 is a top plan view of an end plate for an enclosure for a hydrogen purification device constructed according to the present invention.

FIG. 26 is a side elevation view of the end plate of FIG. 25.

FIG. 27 is a partial cross-sectional side elevation view of an enclosure for a hydrogen purification device constructed with a pair of the end plates shown in FIGS. 25-26.

FIG. 28 is an isometric view of another hydrogen purification device constructed according to the present invention.

FIG. 29 is a cross-sectional view of the device of FIG. 28.

FIG. 30 is a side elevation view of another end plate for a hydrogen purification device constructed according to the present invention.

FIG. 31 is a side elevation view of another end plate for a hydrogen purification device constructed according to the present invention.

FIG. 32 is a side elevation view of another end plate for a hydrogen purification device constructed according to the present invention.

FIG. 33 is a fragmentary side elevation view of a pair of separation membranes separated by a support.

FIG. 34 is an exploded isometric view of a membrane envelope constructed according to the present invention and including a support in the form of a screen structure having several layers.

FIG. 35 is an exploded isometric view of another membrane envelope according to the present invention.

FIG. 36 is an exploded isometric view of another membrane envelope constructed according to the present invention.

FIG. 37 is an exploded isometric view of another membrane envelope constructed according to the present invention.

FIG. 38 is a cross-sectional view of a shell for an enclosure for a hydrogen purification device constructed according to the present invention with an illustrative membrane frame and membrane module shown in dashed lines.

FIG. 39 is a top plan view of the end plate of FIG. 21 with an illustrative separation membrane and frame shown in dashed lines.

FIG. 40 is a top plan view of the end plate of FIG. 25 with an illustrative separation membrane and frame shown in dashed lines.

FIG. 41 is an exploded isometric view of another hydrogen purification device constructed according to the present invention.

FIG. 42 is a schematic diagram of a fuel processing system that includes a fuel processor and a hydrogen purification device constructed according to the present invention.

FIG. 43 is a schematic diagram of a fuel processing system that includes a fuel processor integrated with a hydrogen purification device according to the present invention.

FIG. 44 is a schematic diagram of another fuel processor that includes an integrated hydrogen purification device constructed according to the present invention.

FIG. 45 is a schematic diagram of a fuel cell system that includes a hydrogen purification device constructed according to the present invention.

FIG. 46 is a cross-sectional view showing an example of a steam reformer constructed according to the present invention.

FIG. 47 is a cross-sectional view showing another example of a steam reformer constructed according to the present invention.

FIG. 48 is a cross-sectional view showing another example of a steam reformer constructed according to the present invention.

FIG. 49 is a cross-sectional view showing another example of a steam reformer constructed according to the present invention.

FIG. 50 is a cross-sectional view showing another example of a steam reformer constructed according to the present invention.

FIG. 51 is a cross-sectional view showing another example of a steam reformer constructed according to the present invention.

DETAILED DESCRIPTION AND BEST MODE OF THE DISCLOSURE

A hydrogen purification device is schematically illustrated in FIG. 1 and generally indicated at 10 . Device 10 includes a body, or enclosure, 12 that defines an internal compartment 18 in which a separation assembly 20 is positioned. A mixed gas stream 24 containing hydrogen gas 26 and other gases 28 is delivered to the internal compartment. More specifically, the mixed gas stream is delivered to a mixed gas region 30 of the internal compartment and into contact with separation assembly 20 . Separation assembly 20 includes any suitable structure adapted to receive the mixed gas stream and to produce therefrom a permeate, or hydrogen-rich, stream. Stream 34 typically will contain pure or at least substantially pure hydrogen gas. However, it within the scope of the disclosure that stream 34 may at least initially also include a carrier, or sweep, gas component.

In the illustrated embodiment, the portion of the mixed gas stream that passes through the separation assembly enters a permeate region 32 of the internal compartment. This portion of the mixed gas stream forms hydrogen-rich stream 34 , and the portion of the mixed gas stream that does not pass through the separation assembly forms a byproduct stream 36 , which contains at least a substantial portion of the other gases. In some embodiments, byproduct stream 36 may contain a portion of the hydrogen gas present in the mixed gas stream. It is also within the scope of the disclosure that the separation assembly is adapted to trap or otherwise retain at least a substantial portion of the other gases, which will be removed as a byproduct stream as the assembly is replaced, regenerated or otherwise recharged. In FIG. 1, streams 24 - 28 are meant to schematically represent that each of streams 24 - 28 may include more that one actual stream flowing into or out of device 10 . For example, device 10 may receive plural feed streams 24 , a single stream 24 that is divided into plural streams prior to contacting separation assembly 20 , or simply a single stream that is delivered into compartment 18 .

Device 10 is typically operated at elevated temperatures and/or pressures. For example, device 10 may be operated at (selected) temperatures in the range of ambient temperatures up to 700° C. or more. In many embodiments, the selected temperature will be in the range of 200° C. and 500° C., in other embodiments, the selected temperature will be in the range of 250° C. and 400° C. and in still other embodiments, the selected temperature will be 400° C.±either 25° C., 50° C. or 75° C. Device 10 may be operated at (selected) pressures in the range of approximately 50 psi and 1000 psi or more. In many embodiments, the selected pressure will be in the range of 50 psi and 250 or 500 psi, in other embodiments, the selected pressure will be less than 300 psi or less than 250 psi, and in still other embodiments, the selected pressure will be 175 psi±either 25 psi, 50 psi or 75 psi. As a result, the enclosure must be sufficiently well sealed to achieve and withstand the operating pressure.

It should be understood that as used herein with reference to operating parameters like temperature or pressure, the term “selected” refers to defined or predetermined threshold values or ranges of values, with device 10 and any associated components being configured to operate at or within these selected values. For further illustration, a selected operating temperature may be an operating temperature above or below a specific temperature, within a specific range of temperatures, or within a defined tolerance from a specific temperature, such as within 5%, 10%, etc. of a specific temperature.

In embodiments of the hydrogen purification device in which the device is operated at an elevated operating temperature, heat needs to be applied to, or generated within, the device to raise the temperature of the device to the selected operating temperature. For example, this heat may be provided by any suitable heating assembly 42 . Illustrative examples of heating assembly 42 have been schematically illustrated in FIG. 1. It should be understood that assembly 42 may take any suitable form, including mixed gas stream 24 itself. Illustrative examples of other suitable heating assemblies include one or more of a resistance heater, a burner or other combustion region that produces a heated exhaust stream, heat exchange with a heated fluid stream other than mixed gas stream 24 , etc. When a burner or other combustion chamber is used, a fuel stream is consumed and byproduct stream 36 may form all or a portion of this fuel stream. At 42 ′ in FIG. 1, schematic representations have been made to illustrate that the heating assembly may deliver the heated fluid stream external device 10 , such as within a jacket that surrounds or at least partially surrounds the enclosure, by a stream that extends into the enclosure or through passages in the enclosure, or by conduction, such as with an electric resistance heater or other device that radiates or conducts electrically generated heat.

A suitable structure for separation assembly 20 is one or more hydrogen-permeable and/or hydrogen-selective membranes 46 , such as somewhat schematically illustrated in FIG. 2. As shown, membrane 46 includes a pair of generally opposed surfaces 2 and an edge 4 joining the perimeters of the surfaces. Each surface 2 includes an outer edge region 6 that surrounds a central region 8 . Membrane 46 is typically roll formed and, as shown, has a generally rectangular, sheet-like configuration with a constant thickness. It should be understood that membrane 46 may have any geometric or irregular shape, such as by cutting the formed membrane into a desired shape based on user preferences or application requirements. It is within the scope of the disclosure that any suitable method for forming membrane 46 may be used. For example, membrane 46 may also be formed from such processes as electro deposition, sputtering or vapor deposition.

In FIG. 3, membrane 46 is shown in cross-section, and it can be seen that the thickness 11 of the membrane measured between the central regions is the same as the thickness 13 measured between the edge regions. In the figures, it should be understood that the thicknesses of the membranes and subsequently described absorbent media and frame have been exaggerated for purposes of illustration. Typically, hydrogen-permeable membranes have thicknesses less than approximately 50 microns, although the disclosed etching process may be used with thicker membranes.

Membrane 46 may be formed of any hydrogen-permeable material suitable for use in the operating environment and parameters in which purification device 10 is operated. Examples of suitable materials for membranes 46 include palladium and palladium alloys, and especially thin films of such metals and metal alloys. Palladium alloys have proven particularly effective, especially palladium with 35 wt % to 45 wt % copper. More specific examples of a palladium alloy that have proven effective include palladium-copper alloys containing 40 wt % (+/−0.25 or 0.5 wt %) copper, although other alloys and percentages are within the scope of the disclosure. Membranes 46 are typically formed from a thin foil that is approximately 0.001 inches thick. Accordingly, it should be understood that the thicknesses of the membranes illustrated herein have been exaggerated for purposes of illustration. It is within the scope of the present disclosure, however, that the membranes may be formed from hydrogen-permeable and/or hydrogen-selective materials, including metals and metal alloys other than those discussed above as well as non-metallic materials and compositions.

Metal membranes according to the present disclosure, and especially palladium and palladium alloy membranes, typically will also include relatively small amounts of at least one of carbon, silicon and oxygen, typically ranging from a few parts per million (ppm) to several hundred or more parts per million. For example, carbon may be introduced to the membrane either intentionally or unintentionally, such as from the raw materials from which the membranes are formed and/or through the handling and formation process. Because many lubricants are carbon-based, the machinery used in the formation and processing of the membranes may introduce carbon to the material from which the membranes are formed. Similarly, carbon-containing oils may be transferred to the material by direct or indirect contact with a user's body. Preferably, membranes constructed according to the present disclosure include less than 250 ppm carbon, and more preferably less than 150, 100 or 50 ppm carbon. Nonetheless, the membranes will typically still contain some carbon content, such as at least 5 or 10 ppm carbon. Therefore, it is within the scope of the disclosure that the membranes will contain carbon concentrations within the above ranges, such as approximately 5-150 or 10-150 ppm, 5-100 or 10-100 ppm, or 5-50 or 10-50 ppm carbon.

It is further within the scope of the disclosure that the membranes may include trace amounts of silicon and/or oxygen. For example, oxygen may be present in the Pd40Cu (or other alloy or metal) material in concentrations within the range of 5-200 ppm, including ranges of 5-100, 10-100, 5-50 and 10-50 ppm. Additionally or alternatively, silicon may be present in the material in concentrations in the range of 5-100 ppm, including ranges of 5-10 and 10-50 ppm.

In experiments, reducing the concentration of carbon in the membranes results in an increase in hydrogen flux, compared to a similar membrane that is used in similar operating conditions but which contains a greater concentration of carbon. Similarly, it is expected that increasing the oxygen and/or silicon concentrations will detrimentally affect the mechanical properties of the membrane. The following table demonstrates the correlation between high hydrogen permeability (represented as hydrogen flux through a 25 micron thick membrane at 100 psig hydrogen, 400 degrees Celsius) and low carbon content.

TABLE 1
Hydrogen flux through 25 micron thick Pd—40Cu membranes
containing trace amounts of carbon, oxygen and silicon
at 400° C. and 100 psig hydrogen
	Hydrogen Flux	Concentration (ppm)
	(std ft 3 /ft 2 · hr)	Carbon	Oxygen	Silicon
	130	40	25	10
	125	56	29	39
	115	146	25	15
	56	219	25	27

It is within the scope of the disclosure that the membranes may have a variety of thicknesses, including thicknesses that are greater or less than discussed above. For example, the membrane may be made thinner, with commensurate increase in hydrogen flux. Examples of suitable mechanisms for reducing the thickness of the membranes include rolling, sputtering and etching. A suitable etching process is disclosed in U.S. Pat. No. 6,152,995, the complete disclosure of which is hereby incorporated by reference for all purposes. Examples of various membranes, membrane configurations, and methods for preparing the same are disclosed in U.S. Pat. Nos. 6,221,117 and 6,319,306, the complete disclosures of which are hereby incorporated by reference for all purposes. The above-described “trace” components (carbon, oxygen and/or silicon) may be described as being secondary components of the material from which the membranes are formed, with palladium or a palladium alloy being referred to as the primary component. In practice, it is within the scope of the disclosure that these trace components may be alloyed with the palladium or palladium alloy material from which the membranes are formed or otherwise distributed or present within the membranes.

As discussed, membrane 46 may be formed of a hydrogen-permeable metal or metal alloy, such as palladium or a palladium alloy, including a palladium alloy that is essentially comprised of 60 wt % palladium and 40 wt % copper. Because palladium and palladium alloys are expensive, the thickness of the membrane should be minimal; i.e., as thin as possible without introducing an excessive number of holes in the membrane if it is desirable to reduce the expense of the membranes. Holes in the membrane are not desired because holes allow all gaseous components, including impurities, to pass through the membrane, thereby counteracting the hydrogen-selectivity of the membrane.

An example of a method for reducing the thickness of a hydrogen-permeable membrane is to roll form the membrane to be very thin, such as with thicknesses of less than approximately 50 microns, and more commonly with thicknesses of approximately 25 microns. The flux through a hydrogen-permeable metal membrane is inversely proportional to the membrane thickness. Therefore, by decreasing the thickness of the membrane, it is expected that the flux through the membrane will increase, and vice versa. In Table 2, below, the expected flux of hydrogen through various thicknesses of Pd-40Cu membranes is shown.

TABLE 2
Expected hydrogen flux through Pd—40Cu membranes
at 400° C. and 100 psig hydrogen feed, permeate
hydrogen at ambient pressure.
	Membrane Thickness	Expected Hydrogen Flux
	25 micron	60 mL/cm 2 · min
	17 micron	88 mL/cm 2 · min
	15 micron	100 mL/cm 2 · min

Besides the increase in flux obtained by decreasing the thickness of the membrane, the cost to obtain the membrane also increases as the membrane's thickness is reduced. Also, as the thickness of a membrane decreases, the membrane becomes more fragile and difficult to handle without damaging.

Through the etching process, or method, of the present disclosure, discussed in more detail subsequently, the thickness of a portion of the membrane, such as central region 8 , may be selectively reduced, while leaving the remaining portion of the membrane, such as edge region 6 , at its original thickness. Therefore, greater flux is obtained in the thinner etched region, while leaving a thicker, more durable edge region that bounds the central region and thereby provides support to the membrane.

For example, an etched membrane 46 prepared according to an etching method of the present disclosure is shown in FIG. 4 and illustrated generally at 17 . Similar to the other membranes 46 described and illustrated herein, membrane 17 includes a pair of generally opposed surfaces 19 and an edge 23 joining the surfaces. Each surface 19 includes an outer edge region 25 that surrounds a central region 27 . Membrane 17 is formed from any of the above-discussed hydrogen-permeable metal materials, and may have any of the above-discussed configurations and shapes. The etching process works effectively on work-hardened, or non-annealed membranes. Alternatively, the membrane may be annealed prior to the etching process. Unlike an unetched embodiment of membrane 46 , however, the thickness of membrane 17 measured between central regions 27 is less than the thickness 31 measured between the edge regions, as schematically illustrated in FIG. 5. Therefore, the hydrogen flux through the central region will be greater than that through the edge region, as expected from the above discussion of the inversely proportional relationship between membrane thickness and hydrogen flux.

However, an unexpected benefit of chemically etching the membrane, as disclosed herein, is that the hydrogen flux through the etched region exceeds that expected or measured through roll-formed membranes of equal thickness. As shown below in Table 3, the method of the present disclosure yields a hydrogen-permeable metal membrane with significantly greater flux than unetched membranes of similar thicknesses.

TABLE 3
Hydrogen flux through etched and unetched Pd—40Cu membranes
at 400° C. and 100 psig hydrogen feed, permeate hydrogen
at ambient pressure. Aqua regia etchant.
Etching	Membrane	Observed	Expected
Time	Thickness	Hydrogen Flux	Hydrogen Flux
None	25 micron	60 mL/cm 2 · min	60 mL/cm 2 · min
2.0 mins	17 micron	94 mL/cm 2 · min	88 mL/cm 2 · min
2.5 mins	15 micron	122 mL/cm 2 · min	100 mL/cm 2 · min

As the above table demonstrates, the invented method produces hydrogen-permeable metal membranes that permit increased hydrogen throughput compared to unetched membranes of similar thickness by increasing the roughness and surface area of the etched region of the membrane. Perhaps more importantly, this increase in throughput is achieved without sacrificing selectivity for hydrogen or the purity of the harvested hydrogen gas, which is passed through the membrane.

Increasing the surface roughness of the membrane is especially beneficial as the thickness of the membrane is reduced to less than 25 microns, especially less than 20 microns. As the membrane thickness is reduced, the surface reaction rates governing the transport of gaseous molecular hydrogen onto the surface of the metal membrane become more important to the overall permeation rate of hydrogen across the membrane. In extreme cases in which the membrane is quite thin (less than approximately 15 microns) the surface reaction rates are significant in governing the overall permeation rate of hydrogen across the membrane. Therefore, increasing the surface area increases the rate of hydrogen permeation. This contrasts with relatively thick membranes (greater than 25 microns) in which the surface reaction rates are less important and the overall permeation rate of hydrogen across the membrane is governed by the bulk diffusion of hydrogen through the membrane.

Thus the etching process results in an overall reduction in the thickness of the membrane and an increase in the surface roughness (and surface area) of the membrane. These improvements yield an increase in hydrogen flux and reduce the amount of material (e.g., palladium alloy) that is required, while still maintaining the membrane's selectivity for hydrogen.

In the invented etching process, an etchant is used to selectively reduce the thickness of the membrane. When the etchant removes, or etches, material from the surface of a membrane, the etchant also increases the surface roughness and surface area of the membrane in the etched region.

Examples of suitable etchants include oxidizing agents and acids. An example of a suitable oxidizing acid is nitric acid. Other suitable examples include combinations of nitric acid with other acids, such as aqua regia (a mixture of 25 vol % concentrated nitric acid and 75 vol % concentrated hydrochloric acid). Another specific example of an etchant well-suited to use in the present disclosure is a mixture comprising 67 wt % concentrated nitric acid and 33 wt % aqueous solution of poly(vinyl alcohol). A suitable method of preparing the aqueous solution of poly(vinyl alcohol) is to dissolve 4 wt % of poly(vinyl alcohol) (average molecular weight 124,000 to 186,000; 87% to 89% hydrolyzed; Aldrich Chemical Company, Milwaukee, Wis.) in de-ionized water. The disclosed examples of etchants are for illustrative purposes, and should not be construed to be limiting examples. For example, the relative percentage of acid may be increased or decreased to make the etchant respectively more or less reactive, as desired.

In a first method of the present disclosure, a selected etchant is applied to at least one of the surfaces of the membrane. Once applied, the etchant removes material from the surface of the membrane, thereby increasing its surface roughness and reducing the thickness of the membrane in the etched region. After a defined time period, the etchant is removed. The etching process disclosed herein typically is conducted under ambient conditions (temperature and pressure), although it should be understood that the process could be conducted at elevated or reduced temperatures and pressures as well.

The etching process is limited either by the time during which the membrane is exposed to the etchant, or by the reactive elements of the etchant. In the latter scenario, it should be understood that the etching reaction is self-limiting, in that the reaction will reach an equilibrium state in which the concentration of dissolved membrane in the etchant solution remains relatively constant. Regardless of the limiting factor in the process, it is important to apply a volume and concentration of etchant for a time period that will not result in the etchant creating substantial holes in, or completely dissolving, the membrane. Preferably, no holes are created in the membrane during the etching process.

When applying the etchant to a surface of membrane 46 , such as to produce membrane 17 , it is desirable to control the region of the surface over which the etchant extends. It is also desirable to maintain an even distribution of etchant over this application region. If the application region of the etchant is not controlled, then the etchant may remove material from other non-desired regions of the membrane, such as the edge region, or may damage materials joined to the membrane, such as an attached frame. If an even distribution of etchant is not maintained, areas of increased etchant may have too much material removed, resulting in holes in the membrane. Similarly, other areas may not have enough material removed, resulting in less than the desired reduction in thickness and increase in flux.

To control the distribution of etchant within the desired application region, an absorbent medium is placed on the membrane and defines an application region to be etched. For example, in FIGS. 6 and 7, the absorbent medium is generally indicated at 33 and covers application region 35 of surface 2 . As shown, medium 33 is sized to cover only a central portion of surface 2 , however, it should be understood that medium 33 may be selectively sized to define application regions of any desired size and shape, up to the complete expanse of surface 2 . Typically, however, only a central portion of each surface is treated, leaving an unetched perimeter of greater thickness than the central region. This unetched region, because of its greater thickness, provides strength and support to membrane 46 while still contributing to the hydrogen permeability of the membrane.

Besides being selected to absorb the particular etchant without adversely reacting to the etchant or metal membrane, it is preferable that medium 33 has a substantially uniform absorbency and diffusivity along its length. When medium 33 absorbs and distributes the etchant uniformly along its length, it distributes the etchant evenly across the application region, thereby removing substantially the same amount of material across the entire application region. The benefit of this is not only that some etchant will contact, and thereby remove material from the entire application region, but also that the etchant will be uniformly distributed across the application region. Therefore, medium 33 prevents too much etchant being localized in an area, which would result in too much material being removed. In a region where too much etchant is applied, the excess etchant is drawn away from that region to other areas of the medium where less etchant is applied. Similarly, in a region where too little etchant is applied, the medium draws etchant to that region to produce an even distribution across the medium, and thereby across the application region.

As a result, the reduction of thickness in membrane 46 will be relatively uniform across the application region, and perhaps, more importantly, will be reproducible regardless of the exact rate and position at which the etchant is applied. Therefore, with the same size and type of medium 33 and the same volume of etchant 37 , the resulting reduction in thickness should be reproducible for membranes of the same composition. Of course, it should be understood that etching removes material from the surface of the membrane, thereby resulting in an uneven, rough surface with increased surface area over an unetched surface. Therefore, the exact surface topography will not be seen. However, the average thickness measured across a section of the membrane should be reproducible. For example, in FIG. 5, the average thickness between central regions 27 is indicated with dashed lines.

Because medium 33 essentially defines the bounds of application region 35 , medium 33 should be sized prior to placing it upon the surface to be etched. After placing the medium in the desired position on one of the membrane's surfaces, such as surface 2 shown in FIG. 6, a volume of etchant is applied. In FIG. 6, the applied volume of etchant is schematically illustrated at 37 , with arrows 39 illustrating the absorption and distribution of etchant 37 across medium 33 .

The applied volume of etchant should be no more than a saturation volume of etchant. An absorbent medium can only absorb up to a defined volume of a particular etchant per unit of medium 33 before reaching the saturation point of the medium. Therefore, it is important not to exceed this saturation point. Too much applied etchant will result in unabsorbed etchant pooling on or adjacent to the medium, such as on the upper surface of medium 33 or around the edges of the medium. When excess etchant contacts the surface, it is likely to result in holes in the membrane because more than the desired amount of material is removed. As discussed, if these holes are numerous or large enough, they will render the membrane unusable for hydrogen purification applications, with any holes lowering the purity of the hydrogen passing through the membrane.

Therefore, to prevent too much etchant from being applied, the volume of etchant applied may approach, but should not exceed, the saturation volume of the etchant.

An example of a suitable absorbent medium is a cellulosic material, such as absorbent paper products. A particular example of an absorbent medium that has proven effective are single-fold paper towels manufactured by the Kimberly Clark company. When a three inch by three inch area of such a towel is used, approximately 2.5 mL of etchant may be applied without exceeding the saturation volume of that area. The capillary action of the cellulosic towel both absorbs the applied etchant and distributes the etchant throughout the towel. Other paper and cellulosic materials may be used as well, as long as they meet the criteria defined herein. Absorbent, diffusive materials other than cellulosic materials may be used as well.

After applying the etchant to medium 33 , the etchant is allowed to remove material from the application region for a determined time period. This period is best determined through experimentation and will vary depending on such factors as the composition, thickness and desired thickness of the membrane, the absorbent medium being used, the composition and concentration of etchant, and the temperature at which the etching process is conducted. After this time period has passed, the medium is removed from the membrane, and the application, or treatment area is rinsed with water to remove any remaining etchant. After rinsing, the method may be repeated to etch another surface of the membrane.

Instead of a single etching step on each surface of the membrane, a variation of the above method includes plural etching steps for each surface to be etched. In the first step, a more reactive, or vigorous etchant is used to remove a substantial portion of the material to be removed. In the second step, a less reactive etchant is used to provide a more controlled, even etch across the application region.

As an illustrative example, Pd-40Cu alloy foil was etched first with concentrated nitric acid for 20-30 seconds using the absorbent medium technique described above. After removing the medium and rinsing and drying the membrane, a second etch with a mixture of 20 vol % neat ethylene glycol and the balance concentrated nitric acid was performed for between 1 and 4 minutes. Subsequent etching steps were performed with the glycol mixture to continue to gradually reduce the thickness of the membrane in the application region. Results of etching Pd-40Cu foil using this method are given in the table below.

TABLE 4
Results of etching Pd—40Cu membrane with concentrated nitric
acid for 30 seconds followed by subsequent etches with concentrated
nitric acid diluted with 20% vol ethylene glycol.
Etching Solution	Etching Time	Observations
None (Virgin Pd—40Cu Foil)	N/A	Measures 0.0013
		inches thick
1)	Conc. Nitric Acid	1) 30 seconds	Measures 0.0008 to
2)	20 vol % ethylene	2) 1.5 minutes	0.0009 inches thick,
	glycol/HNO 3		no pin holes
1)	Conc. Nitric Acid	1) 30 seconds	Measures 0.0005 to
2)	20 vol % ethylene	2) 1.5 minutes	0.0006 inches thick,
	glycol/HNO 3		no pin holes
3)	20 vol % ethylene	3) 1.5 minutes
	glycol/HNO 3
1)	Conc. Nitric Acid	1) 30 seconds	Measures 0.0005
2)	20 vol % ethylene	2) 3 minutes	inches thick, no pin
	glycol/HNO 3		holes in membrane
1)	Conc. Nitric Acid	1) 1 minute	Multiple pin holes in
2)	20 vol % ethylene	2) 3 minutes	membrane
	glycol/HNO 3

Other than confining the etching solution to a desired application region, another benefit of using an absorbent medium to control the placement and distribution of the etchant is that the quantity of etchant (or etching solution) that may be applied without oversaturating the medium is limited. Thus, the etching reaction may be self-limiting, depending on the choice of and composition of etchant. For instance, varying the etching time using 33.3 wt % PVA solution/66.7 wt % concentrated HNO ₃ yielded the results shown in the following table. These results indicate that the volume of etchant that is applied at one time may limit the depth of etching, so long as the etchant is not so reactive or applied in sufficient quantity to completely dissolve the application region.

TABLE 5
Results of etching Pd—40Cu membrane with a solution of
33.3 wt % PVA solution/66.7 wt % concentrated nitric acid.
Etching Time	Observations
0	Measures 0.0013 inches thick
3 minutes	Measures 0.0011 inches thick
4 minutes	Measures 0.0011 inches thick
5 minutes	Measures 0.0011 inches thick
6 minutes	Measures 0.0011 inches thick
3 minutes, rinse, 3 minutes	Measures 0.0008 to 0.0009 inches thick
3 minutes, rinse, 3 minutes,	Measures 0.0006 inches thick,
rinse, 3 minutes	multiple pin holes

In a further variation of the etching method, a suitable mask may be applied to the membrane to define the boundaries of the region to be etched. For example, in FIG. 6, instead of using absorbent medium 33 to define application region 35 , a non-absorbent mask could be applied around edge region 25 . Because this mask does not absorb the etchant, it confines the etchant to an application region bounded by the mask. Following etching, the mask is removed. The mask may be applied as a liquid or it may be a film with an adhesive to bond the film to the membrane.

If the chemical etching process is not properly controlled, tiny holes will appear in the membrane. For example, in FIG. 8 membrane 17 is shown with a hole 41 in its central region 27 . Typically, the holes will be very small, however, the size of a particular hole will depend on the concentration and quantity of etchant applied to that region, as well as the time during which the etchant was allowed to etch material from the membrane. Holes, such as hole 41 , reduce the purity of the hydrogen gas harvested through the membrane, as well as the selectivity of the membrane for hydrogen. The probability of holes forming in the membrane during the etching process increases as the thickness of the membrane is reduced. Therefore, there is often a need to repair any holes formed during the etching process.

One method for detecting any such holes is to utilize a light source to identify holes in the membrane. By shining a light on one side of the membrane, holes are detected where light shines through the other side of the membrane. The detected holes may then be repaired by spot electroplating, such as by using a Hunter Micro-Metallizer Pen available from Hunter Products, Inc., Bridgewater, N.J. In FIG. 7, a patch, or plug, 43 is generally indicated in dashed lines and shown repairing hole 41 . Any other suitable method may be used for repairing tiny holes resulting from etching the membrane.

The repairing step of the invented etching process also may be performed using a photolithographic method. In this case a light-sensitive, electrically insulating mask is applied to one surface of the membrane, and then the membrane is irradiated with light of the appropriate wavelength(s) from the opposite side. Any tiny holes that might be present in the membrane will allow the light to pass through the membrane and be absorbed by the light-sensitive mask. Next, the mask is washed to remove irradiated regions of the mask and thereby reveal the bare metal of the membrane. Because only the irradiated regions of the mask are removed, the remaining mask serves as an electrical insulator over the surface of the membrane. Then, all of the spots where the mask has been removed are electroplated or electrolessplated at the same time.

Because the patch, or plug, represents only a minute percentage of the surface area of the membrane, the patch may be formed from a material that is not hydrogen-permeable without the flux through the membrane being noticeably affected. Of course, a hydrogen-permeable and selective patch is preferred. Suitable metals for electroplating to fill or close tiny holes in the palladium-alloy membranes include copper, silver, gold, nickel, palladium, chromium, rhodium, and platinum. Volatile metals such as zinc, mercury, lead, bismuth and cadmium should be avoided. Furthermore, it is preferable that metal applied by plating be relatively free of phosphorous, carbon, sulfur and nitrogen, since these heteroatoms could contaminate large areas of the membrane and are generally known to reduce the permeability of palladium alloys to hydrogen.

In use, membrane 46 provides a mechanism for removing hydrogen from mixtures of gases because it selectively allows hydrogen to permeate through the membrane. The flowrate, or flux, of hydrogen through membrane 46 typically is accelerated by providing a pressure differential between a mixed gaseous mixture on one side of the membrane, and the side of the membrane to which hydrogen migrates, with the mixture side of the membrane being at a higher pressure than the other side.

Because of their extremely thin construction, membranes 46 typically are supported by at least one of a support or frame. Frames, or frame members, may be used to support the membranes from the perimeter regions of the membranes. Supports, or support assemblies, typically support the membranes by extending across and in contact with at least a substantial portion of one or more of the membrane surfaces, such as surfaces 2 or 19 . By referring briefly back to FIG. 3, an illustrative example of a frame, or frame member, is shown and generally indicated at 15 . Frame 15 is secured to a membrane 46 , such as around a portion or the entire edge region 6 . Frame 15 is formed from a more durable material than the membrane and provides a support structure for the membrane. Frame 15 may be secured to one or both surfaces of the membrane. It should be understood that the invented membrane may be formed without frame 15 . In another variation, frame 15 may take the form of a compressible gasket that is secured to the membrane, such as with an adhesive or other suitable structure or process. Compressible gaskets are used to form gas-tight seals around and/or between the membranes.

In FIG. 9, illustrative examples of suitable configurations for membranes 46 are shown. As shown, membrane 46 includes a mixed-gas surface 48 which is oriented for contact by mixed gas stream 24 , and a permeate surface 50 , which is generally opposed to surface 48 . Also shown at 52 are schematic representations of mounts, which may be any suitable structure for supporting and/or positioning the membranes or other separation assemblies within compartment 18 . Mounts 52 may include or be at least partially formed from frames 15 . Alternatively, mounts 52 may be adapted to be coupled to frame 15 to selectively position the membrane within device 10 . The patent and patent applications incorporated immediately above also disclose illustrative examples of suitable mounts 52 . At 46 ′, membrane 46 is illustrated as a foil or film. At 46 ″, the membrane is supported by an underlying support 54 , such as a mesh or expanded metal screen or a ceramic or other porous material. At 46 ′″, the membrane is coated or formed onto or otherwise bonded to a porous member 56 . It should be understood that the membrane configurations discussed above have been illustrated schematically in FIG. 9 and are not intended to represent every possible configuration within the scope of the disclosure.

Supports 54 , frames 15 and mounts 52 should be thermally and chemically stable under the operating conditions of device 10 , and support 54 should be sufficiently porous or contain sufficient voids to allow hydrogen that permeates membrane 46 to pass substantially unimpeded through the support layer. Examples of support layer materials include metal, carbon, and ceramic foam, porous and microporous ceramics, porous and microporous metals, metal mesh, perforated metal, and slotted metal. Additional examples include woven metal mesh (also known as screen) and tubular metal tension springs.

In embodiments of the disclosure in which membrane 46 is a metal membrane and the support and/or frame also are formed from metal, it is preferable that the support or frame is composed of metal that is formed from a corrosion-resistant material. Examples of such materials include corrosion-resistant alloys, such as stainless steels and non-ferrous corrosion-resistant alloys comprised of one or more of the following metals: chromium, nickel, titanium, niobium, vanadium, zirconium, tantalum, molybdenum, tungsten, silicon, and aluminum. These corrosion-resistant alloys have a native surface oxide layer that is chemically and physically very stable and serves to significantly retard the rate of intermetallic diffusion between the thin metal membrane and the metal support layer. Such intermetallic diffusion, if it were to occur, often results in degradation of the hydrogen permeability of the membrane and is undesirable.

Although membrane 46 is illustrated in FIG. 9 as having a planar configuration, it is within the scope of the disclosure that membrane 46 may have non-planar configurations as well. For example, the shape of the membrane may be defined at least in part by the shape of a support 54 or member 56 upon which the membrane is supported and/or formed. As such, membranes 46 may have concave, convex or other non-planar configurations, especially when device 10 is operating at an elevated pressure. As another example, membrane 46 may have a tubular configuration, such as shown in FIGS. 10 and 11.

In FIG. 10, an example of a tubular membrane is shown in which the mixed gas stream is delivered to the interior of the membrane tube. In this configuration, the interior of the membrane tube defines region 30 of the internal compartment, and the permeate region 32 of the compartment lies external the tube. An additional membrane tube is shown in dashed lines in FIG. 10 to represent graphically that it is within the scope of the present disclosure that device 10 may include more than one membrane and/or more than one mixed-gas surface 48 . It is within the scope of the disclosure that device 10 may also include more than two membranes, and that the relative spacing and/or configuration of the membranes may vary.

In FIG. 1, another example of a hydrogen purification device 10 that includes tubular membranes is shown. In this illustrated configuration, device 10 is configured so that the mixed gas stream is delivered into compartment 18 external to the membrane tube or tubes. In such a configuration, the mixed-gas surface of a membrane tube is exterior to the corresponding permeate surface, and the permeate region is located internal the membrane tube or tubes.

The tubular membranes may have a variety of configurations and constructions, such as those discussed above with respect to the planar membranes shown in FIG. 9. For example, illustrative examples of various mounts 52 , supports 54 and porous members 56 are shown in FIGS. 10 and 11, including a spring 58 , which has been schematically illustrated. It is further within the scope of the disclosure that, tubular membranes may have a configuration other than the straight cylindrical tube shown in FIG. 10. Examples of other configurations include U-shaped tubes and spiral or helical tubes.

As discussed, enclosure 12 defines a pressurized compartment 18 in which separation assembly 20 is positioned. In the embodiments shown in FIGS. 9-11, enclosure 12 includes a pair of end plates 60 that are joined by a perimeter shell 62 . It should be understood that device 10 has been schematically illustrated in FIGS. 9-11 to show representative examples of the general components of the device without intending to be limited to geometry, shape and size. For example, end plates 60 typically are thicker than the walls of perimeter shell 62 , but this is not required. Similarly, the thickness of the end plates may be greater than, less than or the same as the distance between the end plates. As a further example, the thickness of membrane 46 has been exaggerated for purposes of illustration.

In FIGS. 9-11, it can be seen that mixed gas stream 24 is delivered to compartment 18 through an input port 64 , hydrogen-rich (or permeate) stream 34 is removed from device 10 through one or more product ports 66 , and the byproduct stream is removed from device 10 through one or more byproduct ports 68 . In FIG. 9, the ports are shown extending through various ones of the end plates to illustrate that the particular location on enclosure 12 from which the gas streams are delivered to and removed from device 10 may vary. It is also within the scope of the disclosure that one or more of the streams may be delivered or withdrawn through shell 62 , such as illustrated in dashed lines in FIG. 10. It is further within the scope of the invention that ports 64 - 68 may include or be associated with flow-regulating and/or coupling structures. Examples of these structures include one or more of valves, flow and pressure regulators, connectors or other fittings and/or manifold assemblies that are configured to permanently or selectively fluidly interconnect device 10 with upstream and downstream components. For purposes of illustration, these flow-regulating and/or coupling structures are generally indicated at 70 in FIG. 9. For purposes of brevity, structures 70 have not been illustrated in every embodiment. Instead, it should be understood that some or all of the ports for a particular embodiment of device 10 may include any or all of these structures, that each port does not need to have the same, if any, structure 70 , and that two or more ports may in some embodiments share or collectively utilize structure 70 , such as a common collection or delivery manifold, pressure relief valve, fluid-flow valve, etc.

Another illustrative example of a suitable configuration for an end plate 60 is shown in FIG. 10. As shown, plate 60 includes input, product and byproduct ports 64 - 68 . Also shown in FIG. 10 is a heating conduit, or passage, 71 through which a stream 73 containing heat transfer fluids, such as streams 24 , 34 or 36 , exhaust gases, etc., may be passed to selectively heat plate 60 and thereby decrease the heating requirements compared to a similarly sized end plate that is formed from a comparable solid slab of material. Especially when passage 71 is adapted to receive a fluid stream 73 other than one of streams 24 and 34 , it is preferable that the passage be isolated relative to ports 64 - 68 . In operation, hot (exhaust) gas passing through plate 60 elevates the temperature of a device that includes plate 60 and thereby reduces the comparative time required to heat the device during start up. Of course, it is within the scope of the disclosure that devices and/or end plates according to the present disclosure may be formed without passage 71 . Similarly, it is