CA2501137A1 - Reforming and hydrogen purification system - Google Patents

Reforming and hydrogen purification system Download PDF

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Publication number
CA2501137A1
CA2501137A1 CA002501137A CA2501137A CA2501137A1 CA 2501137 A1 CA2501137 A1 CA 2501137A1 CA 002501137 A CA002501137 A CA 002501137A CA 2501137 A CA2501137 A CA 2501137A CA 2501137 A1 CA2501137 A1 CA 2501137A1
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Canada
Prior art keywords
hydrogen
reformer
catalyst bed
vessel
unit
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CA002501137A
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French (fr)
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CA2501137C (en
Inventor
Peter David Devries
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Jiangsu Horizon New Energy Technologies Co Ltd
Hyzon Motors Inc
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Individual
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    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
    • C01B3/501—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by diffusion
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
    • C01B3/384—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts the catalyst being continuously externally heated
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
    • C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
    • C01B2203/0233—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a steam reforming step
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0405—Purification by membrane separation
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0405—Purification by membrane separation
    • C01B2203/041—In-situ membrane purification during hydrogen production
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/0811—Methods of heating the process for making hydrogen or synthesis gas by combustion of fuel
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/10—Process efficiency
    • Y02P20/129—Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines

Abstract

A reforming and hydrogen purification system operating with minimal pressure drop for producing free hydrogen from different hydrogen rich fuels includes a hydrogen reforming catalyst bed (7) in a vessel (19) in communication with a core unit containing a hydrogen permeable selective membrane (18). The vessel is located within an insulated inclosure which forms an air inlet passageway and an exhaust passageway on opposite sides of the vessel. Air and raffinate pass through a burner (75) within the air inlet passageway, providing a heated flue gas to heat the catalyst to the reaction temperature needed to generated free hydrogen from the feedstock. The burner flue gas flows laterally over and along the length of the bed between the input and output ends of the bed.
Hydrogen is recovered from the core for use by a hydrogen-consuming device such as a fuel cell. The remaining unrecovered hydrogen in the reformed gases is contained in raffinate and is used to supply process heat via the burner.
The exhaust flue gas and the inlet air supply pass through a recuperator (30) in which the inlet air is heated from the hot exhaust gas. The feedstock-input line is also coupled to the raffinate line and the hydrogen recovery line to preheat the feedstock prior to entry into the catalyst bed.

Claims (55)

1. A reformer for producing purified hydrogen from a pressurized hydrogen rich fuel, comprising a catalyst bed contained in a catalyst unit having a fuel inlet and a spaced reformed fuel outlet, said unit effective to reform the hydrogen rich fuel and produce reformed gas containing hydrogen upon heating of the catalyst bed, a hydrogen permeable purifier member mounted downstream of said catalyst bed and operable to separate and purify the reformed gas into hydrogen and raffinate; and a heating system for said catalyst bed comprising a heat source that generates a continuous flow of hot gases, said heat source directly coupled to the catalyst unit and arranged to pass said hot gases as a continuous flow laterally through the entire length of said catalyst unit between said fuel inlet and said spaced reformed fuel outlet for simultaneous heating of said catalyst bed and said hydrogen rich fuel.
2. The reformer of claim 1 wherein said catalyst unit and said hydrogen permeable purifier member being mounted in coaxial relation where the hydrogen permeable purifier member is operable to receive and remove hydrogen from the reformed gases produced in the catalyst bed.
3. The reformer of claim 2 wherein the catalyst unit is cylindrical with an open inner annular space, the hydrogen permeable purifier member comprises a separate cylindrical unit, and where the hydrogen permeable purifier member unit is resident within the annular space of said catalyst unit.
4. The reformer of claim 3 including a guard member interposed between said catalyst bed and said permeable purifier member to prevent engagement of the catalyst with said member, said guard member constructed with passages facilitating movement of hydrogen through said permeable purifier member.
5. The hydrogen reformer of claim 2 wherein said catalyst unit includes an outer wall of a high heat conducting material, and a plurality of fins secured to the outer wall and extending outwardly of said outer wall, whereby said heating fluid passes over said catalyst unit and engages said fins and said outer wall for heating said catalyst bed.
6. The hydrogen reformer of claim 5 wherein said fins project radially from said outer walls to establish a controlled flow of said flue gas over said catalyst unit.
7. The reformer of claim 1 wherein said catalyst unit includes a length defined by a linear axis, and said hydrogen permeable purifier unit has length corresponding substantially to the length of said catalyst unit and is mounted coaxially on said linear axis.
8. A reformer for separating and purifying hydrogen from a hydrogen rich feedstock comprising:
a linear metallic pressure vessel having a catalyst bed disposed along a linear axis within the pressure vessel for producing hydrogen, said vessel constructed and arranged with a feedstock inlet for introducing pressurized fuel to be reformed to said catalyst bed and a reformed gas outlet, a hydrogen selective membrane positioned downstream of the catalyst bed and operable to receive reformed gas and separate the reformed gas into hydrogen and raffinate, and a heating unit located upstream of said pressure vessel and directly discharging a heated fluid stream through the catalyst bed laterally to the linear axis of the catalyst bed, said heated fluid stream having a length substantially corresponding to the length of the catalyst bed.
9. The reformer of claim 8 where the catalyst-containing linear metallic pressure vessel is a cylinder which also contains said hydrogen selective membrane, and the catalyst bed surrounds the hydrogen selective membrane in coaxial relationship within the vessel.
10. The reformer of claim 8 wherein said membrane removes only a portion of the hydrogen from the reformed gas a purified hydrogen and said raffinate includes some retained hydrogen.
11. The reformer of claim 9 where the feedstock inlet and reformed gas outlet are spaced apart with the catalyst bed therebetween such that the heating fluid stream effectively heats the fuel and catalyst bed to facilitate the production of hydrogen.
12. The reformer of claim 11 wherein said catalyst bed and the hydrogen selective membrane are separated by a guard wall preventing engagement of the catalyst bed with the membrane.
13. The reformer of claim 8 where said heating unit comprises a catalytic burner, and means for passing a mixture of said raffinate and air through said burner and generating said heated fluid stream for heating the vessel.
14. The reformer of claim 9 wherein said vessel has opposite ends, one end being closed and the other end being open, and said reformer further includes a header unit releasably secured to said other end of said vessel in a sealed fashion wherein the feedstock inlet, reformed gas outlet and purified hydrogen all pass through the header unit.
15. The reformer of claim 14 wherein said catalyst bed and the hydrogen selective membrane are separatedly by a guard wall preventing engagement of the catalyst bed with the membrane.
16. The reformer of claim 15 wherein said guard wall is secured to said header unit and forms an inner annular wall for the catalyst bed.
17. The reformer of claim 11 further including an end wall connected to one end of the vessel, said feedstock inlet extending through said end wall into the catalyst bed to discharge the feedstock into the catalyst bed, a hydrogen recovery line extending through the end wall connected to said membrane to recover purified hydrogen and said reformed gas outlet extending through said end wall at a location spaced from said feedstock inlet.
18. The reformer of claim 8 further including a hydrogen exit line communicating with the hydrogen selective membrane, and wherein said pressurized feedstock inlet is coupled in counterflow fashion to at least one of said hydrogen exit line and said reformed gas outlet to preheat said feedstock.
19. The reformer of claim 18 wherein said feedstock inlet is coupled to both said hydrogen exit line and said reformed gas outlet.
20. The reformer of claim 8 wherein said hydrogen selective membrane is formed of a material selected from the group consisting of an inorganic molecular sieve, a pure metal, an alloyed metal, and an inorganic molecular sieve in combination with a pure or alloyed metal.
21. The reformer of claim 8 wherein said hydrogen selective membrane is secured to a porous core and wherein said porous core is formed of a material selected from the group consisting of a porous metallic material, a porous ceramic material, a porous carbon-containing material, or a laminate of said materials.
22. The reformer of claim 8 wherein a methanation catalyst is located on one side of the purifier membrane.
23. The reformer of claim 8 including a series of spaced fins secured to the vessel and projecting outwardly from the vessel, said fins being heat conductive to transmit heat to the vessel for heating of said catalyst bed.
24. The reformer of claim 23 wherein said fins are rectangular fins and define a rectangular outer surface configuration.
25. The reformer of claim 24, including an enclosing means defining a heating passageway over said vessel including a flue gas inlet passageway and a flue gas exhaust passageway to opposite sides of the vessel between said enclosing means.
26. The reformer of claim 23 wherein said fins are uniformly spaced over the length of said vessel to control the heating of said catalyst bed.
27. The reformer of claim 23 wherein said fins are variably spaced over the length of said vessel to produce an asymmetric heat flux in the catalyst bed.
28. The reformer of claim 23 wherein said heating unit comprises a catalytic burner and said catalytic burner is formed as a coating on the surface of the fins.
29. The reformer of claim 13 further including raffinate pressure control means for depressurizing the raffinate, a dispersing member located downstream of said depressurized raffinate for dispersing said depressurized raffinate in air, and means for feeding the raffinate/air mixture to said catalytic burner to supply said heated fluid stream.
30. The reformer of claim 29 wherein the said dispersing member comprises one or more porous members arranged such that the distributed raffinate/air mixture is richer at the feedstock inlet, and the raffinate/air mixture is leaner at the reformed gas outlet resulting in a higher heat flux per unit area in the catalyst bed, near the feedstock inlet than compared to in the catalyst bed near the reformed gas outlet.
31. The reformer of claim 9 wherein said vessel includes a closure wall at one end and an opposite open end, and a header unit releasable connected to and closing the open end of said vessel, a releasable securement means connecting said vessel to the header unit, and a fixed connection of said hydrogen selective membrane to said header unit for permitting separation of the membrane from said vessel and said header for replacement of said membrane or the catalyst bed surrounding the membrane.
32. The reformer of claim 31 including a guard wall connected to said header unit and located between said membrane and said catalyst bed.
33. The reformer of claim 32 wherein said header unit includes a mounting flange secured to said vessel and an end wall releasably secured to said flange, said feedstock inlet extending through said end wall into the catalyst bed to discharge the feedstock into the catalyst bed, a hydrogen recovery line extending through said end wall and in communication with the membrane to recover the hydrogen, and the reformed gas outlet extending through said end wall coupled to the catalyst bed to receive the raffinate from the catalyst bed, and wherein said heating unit includes a burner having a depressurized fuel supply containing said raffinate.
34. The reformer of claim 8 further including a ceramic member having said hydrogen selective membrane secured to its outer surface.
35. The reformer of claim 34 wherein said membrane is a metal member plated on said ceramic member.
36. The reformer of claim 33 wherein said guard wall and said membrane are secured to said releasable end wall for replacement as a unit.
37. The reformer of claim 33 wherein said flange is interconnected in fixed relation to the vessel with a seal located between opposed surfaces of said flange and said end wall to provide a high pressure seal about the open end of said vessel, and said guard wall and said membrane being fixed to said end wall and removable as a unit for replacement of the membrane and guard wall while maintaining the finned outer vessel.
38. The reformer of claim 8 wherein said feedstock inlet includes a conduit arranged in a serpentine path located in the path of said heated fluid stream downstream of said pressure vessel.
39. The reformer of claim 21 wherein said membrane secured to said core has a thickness in the range of 0.1 to 100 microns.
40. The reformer of claim 8 wherein said pressure vessel is mounted within a housing, the housing including a vertical wall dividing said housing into an air inlet passageway including an air inlet chamber on one side of said vertical wall to supply air to heating and unit located upstream of said pressure vessel and defining an exhaust passageway including an exhaust chamber on the opposite side of said wall to discharge exhaust gas from said heating unit.
41. The reformer of claim 40 wherein said inlet and exhaust passageways are constructed and scaled to establish a low pressure flow path of less than 1 psi through the air inlet passageway and the exhaust passageway.
42. The reformer of claim 40 wherein said heating unit comprises a catalytic burner with said inlet air passing through said catalytic burner, said raffinate connected to a fuel dispersing unit located upstream of the burner in the inlet air passageway, said dispersing unit mixes said inlet air with said raffiante and directs said air/raffinate fuel mixture to said catalytic burner for generating said heated fluid stream passing laterally over the pressure vessel to heat the catalyst bed to a desired reaction temperature for production of hydrogen.
43. The reformer of claim 42, including a counterflow exhaust heat recuperating system for heating of the inlet air supply, said recuperating system comprising a plurality of heat transmitting plates formed of thermally conductive material, and each of said plates transversely mounted on said vertical wall and extending across said inlet and exhaust passageways and including a plurality of distributed openings to permit essentially free air flow and exhaust gas flow through said plates, and sealing means between said plates and said vertical wall to prevent mixing exhaust and inlet gas streams, whereby said plates facilitate the flow of heat from the exhaust flue gas stream to the inlet air supply.
44. The reformer of claim 43 where said sealing means comprises a thermally insulating sealing member placed between each of said plates, and where the sealing member is of sufficient width to substantially prevent mixing of the inlet air and exhaust flue gas.
45. The reformer of claim 44 wherein each of said plates is located in a plane perpendicular to the flow of said inlet air supply and said exhaust flue gas.
46. The reformer of claim 8 wherein said pressure vessel includes an outer wall and opposite ends, one end being closed and the other end being open, and said vessel further includes a flange secured to the open end of said outer wall, an outer header bolted to said flange and operable to close the open end of said pressure vessel, said flange and said header having opposed flat surfaces each having a sealing recess in alignment with each other, each of said recesses including an outwardly extended finger aligned with each other, and a seal member located within the aligned recesses and having said fingers forced into sealing engagement therewith upon attachment of the header to the flange.
47. The reformer of claim 46 wherein said seal member is a ductile metal-member.
48. A replaceable core unit for a hydrogen reformer including a vessel defining a chamber for receiving a catalyst bed, one end of said vessel being closed and the other end being open, said core unit comprising a closure member constructed to be releasably attached to said open end of said vessel and forming a wall for closing of said chamber, and a hydrogen permeable membrane core unit projecting into said vessel and secured to said closure member, said membrane core unit defining a chamber for receiving hydrogen formed within said catalyst bed.
49. The replaceable core unit of claim 48, wherein said catalyst bed surrounds a tubular-shaped open inner annulus, and said membrane core unit is positioned within the inner annulus in coaxial relationship with the catalyst bed.
50. The replaceable core unit of claim 49 wherein said membrane core unit includes an outer protective guard overlying and spaced from said hydrogen permeable membrane, said guard being secured to said closure member and preventing the engagement of the catalyst bed with the membrane.
51. A counterflow heat recuperating system for heating of an inlet air supply in a reformer for producing hydrogen having an air inlet chamber and adjacent exhaust flue gas outlet chamber separated by a common wall, said recuperating system comprising a plurality of heat transmitting plates formed of thermally conductive material, each of said plates transversely mounted on said vertical wall and extending across said air inlet chamber and said exhaust flue gas outlet chamber and including a plurality of distributed openings to permit essentially free inlet air flow and exhaust flue gas flow through said plates, and sealing means between said plates and said common wall to prevent mixing exhaust flue gas and inlet air gas streams, whereby said plates facilitate the flow of heat from the exhaust flue gas stream to the inlet air supply.
52. The system of claim 51 where said sealing means comprises a thermally insulating sealing member placed between each of said plates, and where the sealing means comprises a thermally insulating sealing member placed between each of said plates, and where the sealing member is of sufficient width to substantially prevent mixing of the inlet air and exhaust flue gas.
53. The system of claim 52 wherein each of said heat transmitting plates is located in a plane perpendicular to the flow of said inlet air supply and said exhaust flue gas.
54. A method of producing hydrogen comprising the steps of:
reforming a hydrogen rich feedstock by passing the feedstock through a catalyst bed to produce a reformed gas;
separating the reformed gas into hydrogen and raffinate;
heating the catalyst bed to a desired reaction temperature by passing hot gas from a burner in a continuous flow laterally over said catalyst bed;
recycling at least a portion of said raffinate to said burner to use as fuel for said burner; and recovering said hydrogen.
55. The method of claim 54 further including the steps of:
feeding air to said burner, and pre-heating said air by transferring heat from said hot gas at a location downstream from said catalyst bed.
CA2501137A 2002-10-03 2003-10-03 Reforming and hydrogen purification system Expired - Lifetime CA2501137C (en)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
US10/263,949 2002-10-03
US10/263,949 US7341609B2 (en) 2002-10-03 2002-10-03 Reforming and hydrogen purification system
PCT/US2003/031487 WO2004031073A2 (en) 2002-10-03 2003-10-03 Reforming and hydrogen purification system

Publications (2)

Publication Number Publication Date
CA2501137A1 true CA2501137A1 (en) 2004-04-15
CA2501137C CA2501137C (en) 2012-04-24

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CA2501137A Expired - Lifetime CA2501137C (en) 2002-10-03 2003-10-03 Reforming and hydrogen purification system

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US (2) US7341609B2 (en)
EP (1) EP1546031A2 (en)
JP (1) JP4598529B2 (en)
CN (1) CN100411972C (en)
AU (1) AU2003282674A1 (en)
BR (1) BR0314535A (en)
CA (1) CA2501137C (en)
WO (1) WO2004031073A2 (en)

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US20080134577A1 (en) 2008-06-12
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AU2003282674A1 (en) 2004-04-23
JP4598529B2 (en) 2010-12-15

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