CA2439773A1 - Apparatus and process for the production of hydrogen - Google Patents

Apparatus and process for the production of hydrogen Download PDF

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Publication number
CA2439773A1
CA2439773A1 CA002439773A CA2439773A CA2439773A1 CA 2439773 A1 CA2439773 A1 CA 2439773A1 CA 002439773 A CA002439773 A CA 002439773A CA 2439773 A CA2439773 A CA 2439773A CA 2439773 A1 CA2439773 A1 CA 2439773A1
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Prior art keywords
hydrogen
fuel cell
process according
membrane
oxidant
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CA002439773A
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French (fr)
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CA2439773C (en
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Andreas Nikolaos Matzakos
Thomas Mikus
John Michael Ward
Scott Lee Wellington
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Shell Canada Ltd
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Individual
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/22—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by diffusion
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D63/00—Apparatus in general for separation processes using semi-permeable membranes
    • B01D63/06—Tubular membrane modules
    • B01D63/062—Tubular membrane modules with membranes on a surface of a support tube
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
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    • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/008—Details of the reactor or of the particulate material; Processes to increase or to retard the rate of reaction
    • B01J8/009—Membranes, e.g. feeding or removing reactants or products to or from the catalyst bed through a membrane
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    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/0207—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid flow within the bed being predominantly horizontal
    • B01J8/0214—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid flow within the bed being predominantly horizontal in a cylindrical annular shaped bed
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    • B01J8/0242—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid flow within the bed being predominantly vertical
    • B01J8/0257—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid flow within the bed being predominantly vertical in a cylindrical annular shaped bed
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/10—Catalysts for performing the hydrogen forming reactions
    • C01B2203/1041—Composition of the catalyst
    • C01B2203/1047—Group VIII metal catalysts
    • C01B2203/1052—Nickel or cobalt catalysts
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    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
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    • C01B2203/80—Aspect of integrated processes for the production of hydrogen or synthesis gas not covered by groups C01B2203/02 - C01B2203/1695
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    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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Abstract

Disclosed is a new process and apparatus for steam reforming of any vaporizable hydrocarbon to produce H2 and CO2, with minimal CO, and no CO in the H2 stream, using a membrane steam reforming (MSR) reactor and flame-less distributed combustion (FDC) which provides great improvements in heat exchange efficiency and load following capabilities to drive the steam reforming reaction. The invention also pertains to a zero emission hybrid power system wherein the produced hydrogen is used to power a high-pressure internally manifolded molten carbonate fuel cell. In addition, the design of the FDC-MSR powered fuel cell makes it possible to capture good concentratio ns of CO2 for sequestration or use in other processes.

Claims (29)

1. An apparatus for the production of hydrogen compris-ing:
a) a steam reforming reactor comprising two concentric sections including a larger outside section and a smaller inside section and an annulus containing reforming cata-lyst between the sections;
b) the annulus section having an inlet for steam and va-porizable hydrocarbon, a flow path for hydrogen and by-product gases resulting from reforming reactions taking place in the annulus section, and an outlet for the by-product gases;
c) the outside section being in heat transferring con-tact with the annulus section, and having an inlet for preheated air or other oxidant and a plurality of tubes for fuel gas, said tubes having openings through which the fuel gas flows and is mixed with the air or other oxidant resulting in flameless distributed combustion, whereby uniform, controlled heat is transferred to said annulus section;
d) the inside section having an hydrogen-selective, hy-drogen-permeable membrane positioned either on the inside or outside of the inside section, and an outlet for hy-drogen which permeates through the membrane from the an-nulus section into the inside section and passes through the outlet.
2. Apparatus according to claim 1 further comprising a stinger pipe located in the inner section for introducing sweep gas into that section.
3. Apparatus according to claim 1 or 2, wherein the re-forming catalyst comprises at least one Group VIII tran-sition metal on a support, preferably comprises nickel on alumina.
4. Apparatus according to any one of the preceding claims, wherein the hydrogen-permeable selective membrane comprises one or more Group VIII transition metals or al-loys thereof, preferably palladium, platinum or a palla-dium or platinum alloy.
5. Apparatus according to claim 4, wherein the membrane comprises at least one of an alloy of Pd with 30-50 %wt copper, an alloy of Pd with 5-30 %wt silver, an alloy of Pd with 1-10 %wt yttrium, an alloy of Pd with 1-10 %wt holmium, an alloy of Pd with 10 %wt gold, an alloy of Pd with 1-10 %wt ruthenium and an alloy of Pd with 1-10 %wt cerium.
6. Apparatus according to any one of the preceding claims, wherein the hydrogen-permeable membrane is situ-ated on a support, preferably a porous metal or ceramic support.
7. Apparatus according to claim 6, wherein the membrane support provides an intermediate layer between the mem-brane and the catalyst.
8. Apparatus according to any one of the preceding claims, wherein the membrane has a thickness in the range of from 10 Angstroms to 150 µm, preferably of from 0.1 to 20 µm, more preferably of from 0.5 to 10 µm.
9. Apparatus according to any one of the preceding claims, wherein the membrane has a permeability in the range of 8 x 10-4 to 80 standard cubic me-tres/m2/sec/bar0-5, preferably in the range of from 8 x 10-3 to 70 standard cubic metres/m2/sec/bar0-5.
10. Apparatus according to any one of the preceding claims, wherein the steam reforming reactor is constructed of an alloy containing less than 25% Cr and less than 20% Ni, with most of the balance comprising iron, preferably an alloy containing 15 to 20% Cr and 5 to 15% Ni, more preferably AISI 304 stainless steel, comprising about 18% Cr, about 8% Ni, and the most of the balance Fe.
11. Apparatus according to any one of the preceding claims, wherein the inside section is packed with a methanation catalyst.
12. A fuel cell system comprising a fuel cell in communi-cation with the apparatus according to any one of the preceding claims.
13. A fuel cell system according to claim 12, wherein the fuel cell is a high pressure fuel cell, preferably a high pressure molten carbonate fuel cell.
14. A process for the production of hydrogen, comprising:
a) reacting steam with a vaporizable hydrocarbon at a temperature of from about 200 °C to about 700 °C and at a pressure of from about 1 bara to about 200 bara in a reaction zone containing a reforming catalyst to produce a mixture of primarily hydrogen and carbon dioxide, with a lesser amount of carbon monoxide;
b) providing heat to the reaction zone by employing flameless distributed combustion thereby driving the reaction;
c) conducting the reaction in the vicinity of a hydrogen-permeable and hydrogen-selective membrane, whereby hydrogen formed in the reaction zone permeates through the selective membrane and is separated from the carbon dioxide and carbon monoxide produced, wherein the flameless distributed combustion used to drive the reaction comprises:

i) preheating either a fuel gas or oxidant or both to a temperature that exceeds the auto-ignition temperature of the fuel gas and oxidant when they are mixed;
ii) passing the fuel gas and oxidant into a heating zone which is in heat transferring contact along a substantial portion of the reaction zone; and iiii) mixing the fuel gas and oxidant in said heating zone in a manner that auto-ignition occurs, resulting in combustion without high temperature flames, thereby providing uniform, controllable heat over a substantial portion of the heating zone which is in contact with the reaction zone.
15. A process according to claim 14, wherein the fuel gas is passed through a plurality of tubes in the heating zone, the tubes having openings sized and spaced to control the quantity of fuel gas mixed with oxidant at various points along the heating zone.
16. A process according to claim 19 or 15, wherein the oxidant is air, and the air and fuel gas used for flameless distributed combustion are heated to a temperature between about 1000 °F (815 °C) and about 2300 °F (1260 °C).
17. A process according to any one of claims 14 to 16, wherein the fuel gas is mixed with oxidant in increments so that, upon auto-ignition, the temperature of the resulting combustion gas will rise no more than from about 20 °F (11 °C) to about 200 °F (111 °C).
18. A process according to any one of claims 14 to 17, wherein the fuel gas is hydrogen.
19. A process according to claim 18, wherein the oxidant is air and the hydrogen and air are combusted at a stoichiometric ratio of hydrogen to oxygen of 2:1, resulting in a flue gas stream that has a high concentration of nitrogen on a dry basis.
20. A process according to any one of claims 14 to 19, wherein a sweep gas is used to promote the diffusion of hydrogen through the membrane, preferably a sweep gas selected from the group consisting of steam, carbon dioxide, nitrogen and condensable hydrocarbons, more preferably steam.
21. A process according to any one of claims 14 to 20, wherein a vacuum is used to promote the diffusion of hydrogen through the membrane.
22. A process according to any one of claims 14 to 21, wherein the vaporizable hydrocarbon is natural gas, methane, methanol, ethane, ethanol, propane, butane, light hydrocarbons having 1-4 carbon atoms in each molecule, or light petroleum fractions including naphtha, diesel, kerosene, bet fuel or vacuum gas oil, preferably natural gas, methane, methanol or naphtha.
23. A process according to any one of claims 14 to 22, wherein the vaporizable hydrocarbon and steam provides a minimum overall O:C ratio of 2:1, preferably in the range of from 2:1 to 3:1.
24. A process according to any one of claims 14 to 23, wherein the temperature in the reaction zone is from about 300 °C to about 600 °C, preferably of from about 400 °C to about 500 °C, and the pressure is from about 10 bara to about 50 bara.
25. A process according to any one of claims 14 to 24, wherein the apparatus according to any of one of claims 1 to 11 is used.
26. A process for the production of hydrogen according to any one of claims 15 to 25 and the use thereof in generating electricity, wherein the hydrogen produced is directed to the anode of a fuel cell, preferably a high pressure molten carbonate fuel cell.
27. A process according to claim 26, wherein the fuel cell is a high pressure molten carbonate fuel cell and the non permeable by-product gases from the reaction zone are directed to the cathode of the fuel cell.
28. A process according to claim 26, wherein the fuel cell is a high pressure molten carbonate fuel cell, the process further comprising the separation and sequestration of high concentrations of carbon dioxide from the process streams and/or from other external CO2-containing streams.
29. A process according to claim 27 or 28, wherein nitrogen is obtained as a high purity stream from the outlet of the cathode of the molten carbonate fuel cell.
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NO20033904D0 (en) 2003-09-04
AR032947A1 (en) 2003-12-03
NO20033904L (en) 2003-10-31
WO2002070402A2 (en) 2002-09-12
JP2004531440A (en) 2004-10-14
EP1365990A2 (en) 2003-12-03

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