CA2676186A1 - Method and system for producing a hydrogen enriched fuel using microwave assisted methane plasma decomposition on catalyst - Google Patents

Method and system for producing a hydrogen enriched fuel using microwave assisted methane plasma decomposition on catalyst Download PDF

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CA2676186A1
CA2676186A1 CA002676186A CA2676186A CA2676186A1 CA 2676186 A1 CA2676186 A1 CA 2676186A1 CA 002676186 A CA002676186 A CA 002676186A CA 2676186 A CA2676186 A CA 2676186A CA 2676186 A1 CA2676186 A1 CA 2676186A1
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methane
catalyst
hydrogen
gas
product gas
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CA2676186C (en
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Zhonghua John Zhu
Jiuling Chen
Gaoqing Max Lu
Gregory Solomon
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Eden Energy Ltd
Eden Innovations Ltd
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    • 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
    • C01B3/22—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds
    • C01B3/24—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons
    • C01B3/26—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons using catalysts
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    • B01J23/74—Iron group metals
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    • 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
    • C01B3/503—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by diffusion characterised by the membrane
    • C01B3/505—Membranes containing palladium
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    • D01F9/00—Artificial filaments or the like of other substances; Manufacture thereof; Apparatus specially adapted for the manufacture of carbon filaments
    • D01F9/08—Artificial filaments or the like of other substances; Manufacture thereof; Apparatus specially adapted for the manufacture of carbon filaments of inorganic material
    • D01F9/12—Carbon filaments; Apparatus specially adapted for the manufacture thereof
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    • D01F9/1271—Alkanes or cycloalkanes
    • D01F9/1272—Methane
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    • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
    • B01J23/78—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with alkali- or alkaline earth metals
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    • B01J37/16—Reducing
    • B01J37/18—Reducing with gases containing free hydrogen
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    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/34—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation
    • B01J37/349—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of flames, plasmas or lasers
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0266—Processes for making hydrogen or synthesis gas containing a decomposition step
    • C01B2203/0277—Processes for making hydrogen or synthesis gas containing a decomposition step containing a catalytic decomposition step
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    • C01B2203/0465—Composition of the impurity
    • C01B2203/048—Composition of the impurity the impurity being an organic compound
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    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
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    • C01B2203/08—Methods of heating or cooling
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    • C01B2203/1041—Composition of the catalyst
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    • C01B2203/10—Catalysts for performing the hydrogen forming reactions
    • C01B2203/1041—Composition of the catalyst
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    • C01B2203/1052—Nickel or cobalt catalysts
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    • C01B2203/16—Controlling the process
    • C01B2203/1642—Controlling the product
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    • C01B2203/169—Controlling the feed
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    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/32—Hydrogen storage

Abstract

A method for producing a hydrogen enriched fuel includes the steps of providing a flow of methane gas at a selected flow rate, providing a catalyst (56), producing a methane plasma at a negative pressure using microwave irradiation at a selected microwave power, directing the methane plasma over the catalyst (56), and controlling the flow of methane gas and the microwave power to produce a product gas having a selected composition. A system (10) for producing a hydrogen enriched fuel includes a methane gas source (16), a reactor (12) having a reaction chamber (22) containing a catalyst (56), a microwave power source (14) configured to form a methane plasma, and a vacuum pump (78) configured to maintain the reaction chamber (22) at a negative pressure.

Claims (32)

1. A method for producing a hydrogen enriched fuel comprising:
providing a flow of methane gas at a selected flow rate;
providing a catalyst;
irradiating the methane gas under a negative pressure using microwave irradiation at a selected microwave power to form a methane plasma;
directing the methane plasma over the catalyst; and controlling the flow of methane gas and the microwave power to produce a product gas having a selected composition.
2. The method of claim 1 wherein the product gas comprises from about 10%
to 30% hydrogen by volume, and from about 70% to 90% methane by volume.
3. The method of claim 1 wherein the catalyst comprises Ni or a Ni alloy prepared by coprecipitation with high activity and stability.
4. The method of claim 1 wherein the negative pressure is from about 20 mmHg to 200 mmHg and the microwave power is from about 70 W to 140 W.
5. The method of claim 1 further comprising pretreating the catalyst with a hydrogen gas prior to the directing step.
6. The method of claim 1 wherein the directing step is performed in a tube reactor made of a microwave transparent material.
7. The method of claim 1 wherein the directing step is performed with the catalyst placed on a microwave transparent holder configured to allow the methane plasma to pass through the catalyst.
8. The method of claim 1 wherein the methane gas comprises pure methane or natural gas.
9. A method for producing a hydrogen enriched fuel comprising:
forming a methane plasma using microwave irradiation of a methane gas under a negative pressure and at a selected microwave power;
directing the methane plasma over a catalyst; and controlling a flow of the methane plasma and the microwave power to produce a product gas comprising methane and hydrogen in selected volume percentages, and to remove solid carbon from the product gas in the form of solid fibrous carbon.
10. The method of claim 9 wherein the controlling step is performed to produce the product gas with about 10% to 30% hydrogen by volume.
11. The method of claim 9 wherein the controlling step is performed to produce the product gas with from about 70% to 90% methane by volume.
12. The method of claim 9 further comprising processing the product gas to recover substantially pure hydrogen.
13. The method of claim 9 wherein further comprising flowing the product gas under a vacuum pressure through a Pd/Ag membrane to recover substantially pure hydrogen.
14. The method of claim 9 wherein the microwave power is less than 120 W
and the product gas comprises 2% to 3% of C2H2, and negligible amounts of C2H4, C3H6, C3H8 and C3H4.
15. The method of claim 9 wherein the negative pressure is from about 20 mmHg to about 200 mmHg, and the microwave power is from about 70 W to 160 W.
16. The method of claim 9 wherein the catalyst comprises a metal selected from the group consisting of Ni100, Ni81A1, Ni93A1, Ni77Cu16A1, Ni54Cu27A1 and Ni83Mg6A1.
17. A method for producing a hydrogen enriched fuel comprising:

providing a tube reactor having microwave transparent walls in flow communication with a methane source configured to provide a flow of methane through the tube reactor;
irradiating the methane using microwave irradiation at a selected microwave power to produce a flow of methane plasma;
placing a catalyst in the tube reactor in the flow of methane plasma; and forming a product gas by converting a selected volume percentage of the methane to hydrogen by reaction of the methane plasma in contact with the catalyst, the product gas comprising about 10-30% hydrogen, about 70-90% methane.
18. The method of claim 17 further comprising pretreating the catalyst with hydrogen prior to the placing step.
19. The method of claim 17 wherein the forming the product gas step removes solid fibrous carbon from the product gas as a useful by-product.
20. The method of claim 17 wherein the methane plasma comprises CH4, CH3, CH2, CH, C2H2, C2H4, C2H6, H2 and (e-).
21. The method of claim 17 wherein the forming the product gas step includes a reaction on the surface of the catalyst of CH3, CH2 , CH_, or H_, with CH4, C2H2, or C2H4 and C2H6, to produce solid fibrous carbon and hydrogen.
22. The method of claim 17 wherein the microwave power is less than 120 W
and the product gas comprises 2% to 3% of C2H2, and negligible amounts of C2H4, C3H6, C3H8 and C3H4.
23. The method of claim 17 further comprising flowing the product gas under a vacuum pressure through a Pd/Ag membrane to recover substantially pure hydrogen.
24. A system for producing a hydrogen enriched fuel comprising:
a methane gas source configured to provide a methane gas flow;

a reactor having a reaction chamber with microwave transparent walls in flow communication with the methane gas source and with a vacuum pump;
a microwave power source configured to form a methane plasma in the reaction chamber at a negative pressure; and a catalyst in the reaction chamber configured to contact the methane plasma and to initiate a reaction in which a product gas has a selected volumetric percentage of hydrogen and methane.
25. The system of claim 24 wherein the reactor includes a microwave transparent holder configured to hold the catalyst in contact with the methane plasma.
26. The system of claim 24 wherein the reactor comprises a tube reactor.
27. The system of claim 24 further comprising a hydrogen source in flow communication with the reactor configured to provide a flow of hydrogen gas for pretreating the catalyst.
28. The system of claim 24 further comprising an inert gas source in flow communication with the reactor configured to provide a flow of inert gas for purging the reaction chamber.
29. The system of claim 24 wherein the catalyst comprises Ni or a Ni alloy prepared by coprecipitation with high activity and stability.
30. The system of claim 24 wherein the product gas comprises about 10% to 30% hydrogen by volume, and from about 70% to 90% methane by volume.
31. The system of claim 24 further comprising an infrared sensor configured to measure a temperature of the methane plasma.
32. The system of claim 24 further comprising a gas chromatograph configured to analyze a chemical composition of the product gas.
CA2676186A 2007-01-25 2008-01-13 Method and system for producing a hydrogen enriched fuel using microwave assisted methane plasma decomposition on catalyst Active CA2676186C (en)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
US11/657,299 US8021448B2 (en) 2007-01-25 2007-01-25 Method and system for producing a hydrogen enriched fuel using microwave assisted methane plasma decomposition on catalyst
US11/657,299 2007-01-25
PCT/IB2008/000508 WO2008090466A2 (en) 2007-01-25 2008-01-13 Method and system for producing a hydrogen enriched fuel using microwave assisted methane plasma decomposition on catalyst

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CA2676186C CA2676186C (en) 2012-11-13

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US (1) US8021448B2 (en)
EP (1) EP2106385B1 (en)
JP (1) JP2010516609A (en)
KR (1) KR20090118940A (en)
CN (1) CN101679026A (en)
AU (1) AU2008208613B2 (en)
BR (1) BRPI0806409A2 (en)
CA (1) CA2676186C (en)
MX (1) MX2009007795A (en)
MY (1) MY147169A (en)
NZ (1) NZ578552A (en)
RU (1) RU2427527C2 (en)
WO (1) WO2008090466A2 (en)
ZA (1) ZA200905725B (en)

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