CA2445615A1 - Hydrogen generation apparatus and method for using same - Google Patents

Hydrogen generation apparatus and method for using same Download PDF

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Publication number
CA2445615A1
CA2445615A1 CA002445615A CA2445615A CA2445615A1 CA 2445615 A1 CA2445615 A1 CA 2445615A1 CA 002445615 A CA002445615 A CA 002445615A CA 2445615 A CA2445615 A CA 2445615A CA 2445615 A1 CA2445615 A1 CA 2445615A1
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Prior art keywords
hydrogen
accordance
reaction
combustion
channels
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CA002445615A
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French (fr)
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CA2445615C (en
Inventor
Michael Roy Powell
Charles J. Call
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Intelligent Energy Inc
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Mesosystems Technology, Inc.
Michael Roy Powell
Charles J. Call
Mesofuel, Inc.
Intelligent Energy, Inc.
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    • 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
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    • 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
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • 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
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
    • C01B2203/1217—Alcohols
    • C01B2203/1223—Methanol
    • 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
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
    • C01B2203/1235—Hydrocarbons
    • 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
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
    • C01B2203/1235—Hydrocarbons
    • C01B2203/1241—Natural gas or methane
    • 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
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1288—Evaporation of one or more of the different feed components
    • 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
    • C01B2203/14—Details of the flowsheet
    • C01B2203/146—At least two purification steps in series
    • 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
    • C01B2203/16—Controlling the process
    • 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
    • C01B2203/16—Controlling the process
    • C01B2203/1604—Starting up the process
    • 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
    • Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
    • 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

Abstract

A compact hydrogen generator for use with fuel cells and other applications includes a hydrogen membrane reactor (12) having a combustion chamber and a reaction chamber. The two chambers have a fluid connection and a heat exchan ge relationship with one another. The hydrogen generation apparatus also includ es a fuel supply (14), a fuel supply line (20) for transporting fuel from the fuel supply (14) to the reaction chamber, an oxygen supply (16), an oxygen supply line (22) for transporting oxygen from the oxygen supply (16) to the combustion chamber, as well as a tail gas supply line (23) for transporting tail gases from the reaction chamber, a combustion by-product line (24) for tansporting combustion by-products from the combustion chamber, and a reacti on product line (26) for transporting hydrogen from the reaction chamber.</SDOA B>

Claims (47)

1. A hydrogen generator comprising:
a hydrogen membrane reactor having a combustion chamber in a fluid connection with and a heat exchange relationship with a reaction chamber;
a fuel supply;
a fuel supply line for transporting fuel from the fuel supply to the reaction chamber;
an oxygen supply;
an oxygen supply line for transporting oxygen from the oxygen supply to the combustion chamber;
a tail gas supply line for transporting tail gases from the reaction chamber;
a combustion by-product line for transporting combustion by-products from the combustion chamber; and a reaction product line for transporting hydrogen from the reaction chamber.
2. A hydrogen generator in accordance with claim 1 wherein the hydrogen membrane reactor comprises a top plate, a bottom plate, and a separation plate having first and second opposing surfaces, the top plate and the first surface of the separation plate together defining the reaction chamber, the bottom plate and the second surface of the separation plate together defining the combustion chamber, a hydrogen separation membrane having first and second opposing surfaces disposed between the top plate and the separation plate, the top plate and the first surface of the hydrogen separation membrane together defining a hydrogen exhaust zone and the separation plate and the second surface of the hydrogen separation membrane together defining a reaction zone and wherein the fuel supply line is for transporting fuel to the reaction zone, the tail gas supply line is for transporting tail gas from the reaction zone, and the reaction product line is for transporting hydrogen from the hydrogen exhaust zone.
3. A hydrogen generator in accordance with claim 2 wherein the combustion chamber comprises a plurality of combustion channels extending radially from the surface of the separation plate, the combustion channels creating a fluid path through the combustion chamber;

the hydrogen exhaust zone comprises a plurality of hydrogen exhaust channels extending radially from the first surface of the hydrogen membrane, creating a fluid path through the hydrogen exhaust zone; and the reaction zone comprises a plurality of reaction channels extending radially from the second surface of the hydrogen membrane, creating a fluid path through the reaction zone.
4. A hydrogen generator in accordance with claim 3 wherein the height and width of each of the combustion channels, the hydrogen exhaust channels, and the reaction channels is between 0.01 mm and 10 mm.
5. A hydrogen generator in accordance with claim 3 wherein the height and width of each of the combustion channels, the hydrogen exhaust channels, and the reaction channels is between 0.5 mm and 5 mm.
6. A hydrogen generator in accordance with claim 2 wherein the tail gas supply line makes a fluid connection between the reaction zone and the combustion chamber.
7. A hydrogen generator in accordance with claim 2 wherein the tail gas supply line makes a fluid connection between the reaction zone and the oxygen supply line.
8. A hydrogen generator in accordance with claim 1 further comprising a fuel heat exchanger operably connected to the fuel supply line and one of the combustion by-product line or the reaction product line.
9. A hydrogen generator in accordance with claim 9 wherein the fuel heat exchanger is a counterflow-type heat exchanger.
10. A hydrogen generator in accordance with claim 10 wherein the fuel heat exchanger is a stacked-plate-type heat exchanger having channels with a height and a width between about 0.01 mm and 10 mm running between the stacked plates.
11. A hydrogen generator in accordance with claim 1 further comprising an oxygen heat exchanger operably connected to the oxygen supply line and one of the combustion by-product line or the reaction product supply line.
12. A hydrogen generator in accordance with claim 12 wherein the oxygen heat exchanger is a counterflow-type heat exchanger.
13. A hydrogen generator in accordance with claim 13 wherein the oxygen heat exchanger is a stacked-plate-type heat exchanger having channels with a height and a width between about 0.01 mm and 10 mm running between the stacked plates.
14. A hydrogen generator in accordance with claim 1 further comprising a fuel heat exchanger operably connected to the fuel supply line and the combustion by-product line and an oxygen heat exchanger operably connected to the oxygen supply line and the reaction product supply line.
15. A hydrogen generator in accordance with claim 1 further comprising a hydrogen reservoir in fluid connection with the reaction product supply line.
16. A hydrogen generator in accordance with claim 1 further comprising a hydrogen fuel cell in fluid connection with the reaction product supply line.
17. A hydrogen generator in accordance with claim 1 wherein the fuel supply is an ammonia supply.
18. A hydrogen generator in accordance with claim 1 further comprising a combustion catalyst in the combustion chamber.
19. A hydrogen generator in accordance with claim 2 further comprising a combustion catalyst packed in or coated on the internal surfaces of the combustion channels.
20. A hydrogen generator in accordance with claim 1 further comprising a reaction catalyst in the reaction chamber.
21. A hydrogen generator in accordance with claim 21 further comprising a reaction catalyst packed in or coated on the internal surfaces of the reaction channels.
22. A hydrogen generator in accordance with claim 18 further comprising an ammonia adsorbent supply in fluid communication with the reaction product line.
23. A hydrogen generator in accordance with claim 1 wherein the fuel supply is a hydrocarbon supply.
24. A hydrogen generator in accordance with claim 24 wherein the hydrocarbon supply is methanol, propane, butane, or kerosene supply.
25. A hydrogen membrane reactor comprising a top plate, a bottom plate, and a separation plate having first and second opposing surfaces, the top plate and the first surface of the separation plate together defining the reaction chamber, the bottom plate and the second surface of the separation plate together defining the combustion chamber, the combustion chamber having a plurality of combustion channels extending radially from the surface of the separation plate, the combustion channels creating a fluid path through the combustion chamber, a hydrogen separation membrane having first and second opposing surfaces disposed between the top plate and the separation plate, the top plate and the first surface of the hydrogen separation membrane together defining a hydrogen exhaust zone, the hydrogen exhaust zone having a plurality of hydrogen exhaust channels extending radially from the first surface of the hydrogen membrane, the hydrogen exhaust channels creating a fluid path through the hydrogen exhaust zone, and the separation plate and the second surface of the hydrogen separation membrane together defining a reaction zone;
the reaction zone having a plurality of reaction channels extending radially from the second surface of the hydrogen membrane, the reaction channels creating a fluid path through the reaction zone;
a fuel inlet into the reaction zone;

an oxygen inlet into the combustion chamber;
a tail gas outlet out of the reaction zone;
a hydrogen outlet out of the hydrogen exhaust zone; and a by-product outlet out of the combustion chamber.
26. A hydrogen membrane reactor in accordance with claim 26 wherein the height and width of each of the combustion channels, the hydrogen exhaust channels, and the reaction channels is between 0.01 mm and 10 mm.
27. A hydrogen membrane reactor in accordance with claim 27 wherein the height and width of each of the combustion channels, the hydrogen exhaust channels, and the reaction channels is between 0.5 mm and 5 mm.
28. A hydrogen membrane reactor in accordance with claim 26 further comprising a combustion catalyst packed in or coated on the internal surfaces of the combustion channels.
29. A hydrogen membrane reactor in accordance with claim 26 further comprising a reaction catalyst packed in or coated on the internal surfaces of the reaction channels.
30. A method for generating hydrogen comprising the steps of a. flowing a hydrogen-producing fuel through a reaction zone and into a combustion chamber of a hydrogen membrane reactor, the combustion chamber in fluid connection with and in a heat exchange relationship with a reaction chamber, the reaction chamber including the reaction zone and containing a reaction catalyst initially at a temperature less than the reaction catalyst's light-off temperature and the reaction zone separated from a hydrogen exhaust zone by a hydrogen separation membrane;
combusting the hydrogen-producing fuel to produce combustion by-products while raising the temperature of the reaction catalyst in the reaction zone and exhausting the by-products b. continuing step a for a period of time sufficient to raise the temperature of the reaction catalyst to above its light off temperature;
31 c. flowing additional hydrogen-producing fuel into the reaction chamber, d. reacting the additional hydrogen-producing fuel to produce hydrogen and tail gases;
and separating the hydrogen from the tail gases by selectively passing the hydrogen through the hydrogen membrane.
31. The method in accordance with claim 31 wherein the combustion chamber contains a combustion catalyst having a light-off temperature.
32. The method in accordance with claim 31 wherein the reaction catalyst has a light off temperature of less than 650° C.
33. The method in accordance with claim 32 wherein the combustion catalyst and the reaction catalyst each have a light off temperature of less than 650°
C.
34. The method in accordance with claim 31 further comprising recirculating the tail gas from the reaction zone into the combustion chamber.
35. The method in accordance with claim 31 further comprising preheating the hydrogen-producing fuel prior to flowing the hydrogen producing fuel into the reaction zone.
36. The method in accordance with claim 31 further comprising flowing oxygen into the combustion chamber.
37. The method in accordance with claim 31 further comprising flowing preheated oxygen into the combustion chamber.
38. The method in accordance with claim 37 further comprising flowing preheated oxygen into the combustion chamber.
39. The method in accordance with claim 31 further comprising flowing the separated hydrogen into a hydrogen reservoir.
40. The method in accordance with claim 31 further comprising flowing the separated hydrogen into a a hydrogen fuel cell.
41. The method in accordance with claim 31 wherein the hydrogen-producing fluid is ammonia.
42. The method in accordance with claim 42 further comprising flowing the separated hydrogen through an ammonia adsorbent.
43. The method in accordance with claim 43 wherein the reaction catalyst is a ruthenium catalyst, a nickel catalyst, an iron oxide catalyst, a rhodium catalyst, an iridium catalyst or a rhenium catalyst.
44. The method in accordance with claim 32 wherein the combustion catalyst is a platinum-rhodium catalyst.
45. The method in accordance with claim 31 wherein the hydrogen-producing fluid is a hydrocarbon.
46. The method in accordance with claim 31 wherein the hydrocarbon is methanol, propane, butane or kerosene.
47. A hydrogen generator comprising:
a hydrogen membrane reactor including a combustion chamber having an inlet and an outlet in a heat exchange relationship with a reaction chamber having an inlet and an outlet;
a fuel supply;
a fuel supply line fluidly connecting the fuel supply to the reaction chamber inlet;
an oxygen supply;
an oxygen supply line fluidly connecting the oxygen supply to the combustion chamber inlet;
a tail gas supply line making a fluid connection with the reaction chamber outlet;

a combustion by-product line making a fluid connection with for transporting combustion by-product from the combustion chamber; and a reaction product line for transporting hydrogen from the reaction chamber.
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ATE525327T1 (en) 2011-10-15
EP1390289A2 (en) 2004-02-25
US20050172556A1 (en) 2005-08-11
US7811529B2 (en) 2010-10-12
EP1390289A4 (en) 2009-03-11
ES2386624T3 (en) 2012-08-23
WO2002086987A3 (en) 2003-04-17
HK1063457A1 (en) 2004-12-31
CA2445615C (en) 2011-06-14
WO2002086987A2 (en) 2002-10-31
EP1390289B1 (en) 2011-09-21
AU2002258962A1 (en) 2002-11-05

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