CA2458314A1 - Steam reformer with internal hydrogen purification - Google Patents
Steam reformer with internal hydrogen purification Download PDFInfo
- Publication number
- CA2458314A1 CA2458314A1 CA002458314A CA2458314A CA2458314A1 CA 2458314 A1 CA2458314 A1 CA 2458314A1 CA 002458314 A CA002458314 A CA 002458314A CA 2458314 A CA2458314 A CA 2458314A CA 2458314 A1 CA2458314 A1 CA 2458314A1
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- hydrogen
- stream
- reformer
- membrane
- reforming
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- Hydrogen, Water And Hydrids (AREA)
- Separation Using Semi-Permeable Membranes (AREA)
Abstract
A steam reformer includes a shell, a reforming region within the shell, and a hydrogen purification module. The shell has an outer surface and is adapted to receive a reforming feedstock containing water and at least one of a hydrocarbon and an alcohol. The reforming region within the shell includes a reforming catalyst bed adapted to receive the feedstock and convert the feedstock into a reforming product stream including hydrogen, carbon monoxide and carbon dioxide. The hydrogen purification module includes a hydrogen-selective membrane in fluid communication with the reforming catalyst bed. The membrane is adapted to produce a permeate stream comprised of a portion of the reforming product stream which passes through the membrane, and a byproduct stream comprised of a portion of the reforming product stream which does not pass through the membrane. The hydrogen-selective membrane includes palladium, copper and silicon, and contains no more than 39 ppm silicon.
Claims (77)
1. A steam reformer, comprising:
a shell having an outer surface and being adapted to receive a reforming feedstock containing water and at least one of a hydrocarbon and an alcohol;
a reforming region within the shell and including a reforming catalyst bed adapted to receive the feedstock and convert the feedstock into a reforming product stream comprising hydrogen, carbon monoxide and carbon dioxide; and a hydrogen purification module including a hydrogen-selective membrane in fluid communication with the reforming catalyst bed and adapted to produce a permeate stream comprised of a portion of the reforming product stream which passes through the membrane, and a byproduct stream comprised of a portion of the reforming product stream which does not pass through the membrane, wherein the hydrogen-selective membrane comprises palladium, copper and silicon, and further wherein the hydrogen-selective membrane contains no more than 39 ppm silicon.
a shell having an outer surface and being adapted to receive a reforming feedstock containing water and at least one of a hydrocarbon and an alcohol;
a reforming region within the shell and including a reforming catalyst bed adapted to receive the feedstock and convert the feedstock into a reforming product stream comprising hydrogen, carbon monoxide and carbon dioxide; and a hydrogen purification module including a hydrogen-selective membrane in fluid communication with the reforming catalyst bed and adapted to produce a permeate stream comprised of a portion of the reforming product stream which passes through the membrane, and a byproduct stream comprised of a portion of the reforming product stream which does not pass through the membrane, wherein the hydrogen-selective membrane comprises palladium, copper and silicon, and further wherein the hydrogen-selective membrane contains no more than 39 ppm silicon.
2. The reformer of claim l, wherein the reformer further includes a polishing catalyst bed including a methanation catalyst, wherein the polishing catalyst bed is in fluid communication with the hydrogen purification module and is adapted to receive the permeate stream therefrom and reduce the concentration of carbon dioxide and carbon monoxide in the permeate stream by catalytic reaction to produce methane.
3. The reformer of any one of claims 1 and 2, wherein the reformer is adapted to receive a liquid-phase feedstock and vaporize the feedstock prior to delivery to the reforming catalyst bed.
4. The reformer of any one of claims 1-3, wherein the reforming region includes a plurality of reforming catalyst beds within the shell.
5. The reformer of any one of claims 1-4, wherein the hydrogen-selective membrane is tubular.
6. The reformer of any one of claims 1-5, wherein the reforming catalyst bed at least partially surrounds the hydrogen-selective membrane.
7. The reformer of any one of claims 1-6, wherein the amount of hydrogen in the product stream is less than a theoretically available amount of hydrogen.
8. The reformer of claim 7, wherein the amount of hydrogen in the product stream is between approximately 50% and approximately 80% of the theoretically available amount of hydrogen.
9. The reformer of any one of claims 1-8, wherein the reformer further includes a combustion chamber adapted to receive and combust a fuel stream with an air stream to generate heat for heating the reformer.
10. The reformer of claim 9, wherein the fuel stream is at least partially comprised of the byproduct stream.
11. The reformer of claim 10, wherein the byproduct stream contains sufficient hydrogen to provide, when combusted with air, sufficient heat to maintain the reforming catalyst bed at or above a selected operating temperature.
12. The reformer of any one of claims 9-11, wherein the reformer further includes a polishing catalyst bed located at least substantially within the combustion chamber, wherein the polishing catalyst bed includes a methanation catalyst, and further wherein the polishing catalyst bed is in fluid communication with the hydrogen purification module and is adapted to receive the permeate stream therefrom and reduce the concentration of carbon dioxide and carbon monoxide in the permeate stream by catalytic reaction to produce methane.
13. The reformer of any one of claims 9-12, wherein the combustion chamber receives air for supporting combustion from a cathode air stream discharged from a fuel cell.
14. The reformer of any one of claims 9-13, wherein the reforming feedstock is preheated prior to passage into the reforming region by heat exchange with at least one of the product stream and an exhaust stream from the combustion chamber.
15. The reformer of any one of claims 1-14, further comprising a heater adapted to heat the reforming catalyst bed to a selected operating temperature.
16. The reformer of any one of claims 1-15, wherein the hydrogen-selective membrane further comprises carbon, with the carbon present in the hydrogen-selective membrane in a concentration of no more than 146 ppm.
17. The reformer of claim 16, wherein the hydrogen-selective membrane includes no more than 56 ppm carbon.
18. The reformer of claim 17, wherein the hydrogen-selective membrane contains less than 40 ppm carbon.
19. The reformer of any one of claims 1-18, wherein silicon is present in the hydrogen-selective membrane in a concentration of no more than 15 ppm.
20. The reformer of any one of claims 1-19, wherein the hydrogen-selective membrane further contains oxygen, and further wherein the oxygen is present in the hydrogen-selective membrane in a concentration of no more than 25 ppm.
21. The reformer of any one of claims 1-20, wherein the hydrogen-selective membrane contains approximately 40 wt% copper.
22. The reformer of any one of claims 1-21, wherein the hydrogen-selective membrane is formed from an alloy containing palladium and approximately 40 wt% copper, has a thickness of 25 microns and is adapted to permit a hydrogen flux of at least 130 std. ft3/ft2.cndot.hr through the membrane at 400° C and 100 psig hydrogen.
23. The reformer of any one of claims 1-22, wherein the reformer includes a plurality of the hydrogen-selective membranes.
24. The reformer of any one of claims 1-23, wherein the hydrogen-selective membrane includes a permeate surface and further wherein the hydrogen purification module includes a support adapted to support the permeate surface of the hydrogen-selective membrane.
25. The reformer of claim 24, wherein the support is formed from at least one of the group consisting of metal, carbon, ceramic foam, porous ceramic, microporous ceramic, porous metal, microporous metal, metal mesh, perforated metal, metal screen, metal spring, corrosion-resistant metal, and slotted metal.
26. The reformer of any one of claims 1-25, further comprising a reforming catalyst bed downstream from the hydrogen purification module.
27. The reformer of any one of claim 1-26, wherein the at least one of a hydrocarbon and an alcohol in the reforming feedstock is selected to be nonflammable under the operating conditions of the steam reformer.
28. The reformer of claim 27, wherein the at least one of a hydrocarbon and an alcohol in the reforming feedstock is selected from the group consisting of polyhydroxyl alcohols, polyethers, ethylene glycol, propylene glycol, glycol ethers of ethylene glycol and glycol ethers of propylene glycol.
29. The reformer of claim 27, wherein the at least one of a hydrocarbon and an alcohol in the reforming feedstock has a vapor pressure of less than 100 torr at 100° C.
30. A process for producing hydrogen containing concentrations of carbon monoxide and carbon dioxide below a defined minimum level, the process comprising:
receiving a reforming feedstock containing water and at least one of a hydrocarbon and an alcohol;
delivering the reforming feedstock to a reforming catalyst bed to produce a reforming product stream comprising hydrogen, carbon monoxide and carbon dioxide; and passing the reforming product stream to a hydrogen purification module containing a hydrogen-selective membrane to produce a permeate stream comprising the reforming product stream which passes through the membrane, and a byproduct stream comprising the reforming product stream not passed through the membrane, wherein the hydrogen-selective membrane comprises palladium, copper and silicon, and further wherein the silicon is present in the membrane in a concentration of no more than 39 ppm.
receiving a reforming feedstock containing water and at least one of a hydrocarbon and an alcohol;
delivering the reforming feedstock to a reforming catalyst bed to produce a reforming product stream comprising hydrogen, carbon monoxide and carbon dioxide; and passing the reforming product stream to a hydrogen purification module containing a hydrogen-selective membrane to produce a permeate stream comprising the reforming product stream which passes through the membrane, and a byproduct stream comprising the reforming product stream not passed through the membrane, wherein the hydrogen-selective membrane comprises palladium, copper and silicon, and further wherein the silicon is present in the membrane in a concentration of no more than 39 ppm.
31. The process of claim 30, further comprising passing the permeate stream through a polishing catalyst bed containing a methanation catalyst to convert at least a substantial portion of the carbon monoxide and the carbon dioxide in the permeate stream into methane.
32. The process of any one of claims 30 and 31, wherein the receiving step includes receiving a liquid-phase reforming feedstock, and the process further comprises vaporizing the reforming feedstock prior to delivering the feedstock to the reforming catalyst bed.
33. The process of any one of claims 30-32, further comprising preheating the reforming feedstock prior to the delivering step by heat exchange with at least of the product stream and an exhaust stream from a combustion chamber.
34. The process of any one of claims 30-33, further comprising combusting the byproduct stream with air to heat and maintain the reforming catalyst bed within a selected operating temperature range.
35. The process of any one of claims 30-34, wherein between 50 percent and 80 percent of a theoretically available amount of hydrogen is recovered as the reforming product stream and the remaining amount of the theoretically available amount of hydrogen is withdrawn as a portion of the byproduct stream.
36. The process of any one of claims 30-35, wherein the remaining amount of hydrogen in the byproduct stream is mixed with air and combusted to heat the reforming catalyst bed.
37. The process of any one of claims 30-36, wherein the hydrogen-selective membrane contains no more than 15 ppm silicon.
38. The process of any one of claims 30-36, wherein the hydrogen-selective membrane further contains carbon, with the carbon being present in the hydrogen-selective membrane in a concentration of no more than 146 ppm carbon.
39. The process of claim 38, wherein the hydrogen-selective membrane contains less than 56 ppm carbon.
40. The process of claim 39, wherein the hydrogen-selective membrane contains less than 40 ppm carbon.
41. The process of any one of claims 30-40, wherein the hydrogen-selective membrane further contains oxygen, and further wherein the oxygen is present in the hydrogen-selective membrane in a concentration of no more than 25 ppm.
42. The process of any one of claims 30-41, wherein the hydrogen-selective membrane contains approximately 40 wt% copper.
43. A hydrogen purification device, comprising:
an enclosure defining an internal compartment; wherein the enclosure includes at least one input port through which a mixed gas stream containing hydrogen gas and other gases is delivered to the enclosure, at least one product output port through which a permeate stream containing at least substantially pure hydrogen gas is removed from the enclosure, and at least one byproduct output port through which a byproduct stream containing at least a substantial portion of the other gases is removed from the enclosure; and at least one hydrogen-selective membrane within the compartment, wherein the at least one hydrogen-selective membrane includes a first surface adapted to be contacted by the mixed gas stream and a permeate surface generally opposed to the first surface, wherein the permeate stream is formed from a portion of the mixed gas stream that passes through the at least one hydrogen-selective membrane to the permeate surface, and the byproduct stream is formed from a portion of the mixed gas stream that does not pass through the at least one hydrogen-selective membrane, wherein the membrane is substantially comprised of a primary component selected from a group consisting essentially of palladium and a palladium alloy, and further wherein the membrane further comprises a secondary component consisting of silicon, with the silicon present in the membrane in a concentration of less than approximately 39 ppm.
an enclosure defining an internal compartment; wherein the enclosure includes at least one input port through which a mixed gas stream containing hydrogen gas and other gases is delivered to the enclosure, at least one product output port through which a permeate stream containing at least substantially pure hydrogen gas is removed from the enclosure, and at least one byproduct output port through which a byproduct stream containing at least a substantial portion of the other gases is removed from the enclosure; and at least one hydrogen-selective membrane within the compartment, wherein the at least one hydrogen-selective membrane includes a first surface adapted to be contacted by the mixed gas stream and a permeate surface generally opposed to the first surface, wherein the permeate stream is formed from a portion of the mixed gas stream that passes through the at least one hydrogen-selective membrane to the permeate surface, and the byproduct stream is formed from a portion of the mixed gas stream that does not pass through the at least one hydrogen-selective membrane, wherein the membrane is substantially comprised of a primary component selected from a group consisting essentially of palladium and a palladium alloy, and further wherein the membrane further comprises a secondary component consisting of silicon, with the silicon present in the membrane in a concentration of less than approximately 39 ppm.
44. The device of claim 43, wherein the secondary component contains silicon present in a concentration of less than 15 ppm.
45. The device of claim 43, wherein the secondary component contains silicon in the range of 10-39 ppm.
46. The device of any one of claims 43-45, wherein the secondary component forms an alloy with the primary component.
47. The device of any one of claims 43-46, wherein the primary component includes an alloy of palladium and copper.
48. The device of any one of claims 43-47, wherein the primary component includes an alloy containing palladium and approximately 40 wt%
copper.
copper.
49. The device of any one of claims 43-48, wherein the membrane further comprises carbon, with the carbon being present in the membrane in a concentration of no more than 146 ppm.
50. The device of claim 49, wherein the membrane further comprises carbon in a concentration of no more than 56 ppm.
51. The device of any one of claims 43-50, further comprising a support adapted to support the at least one hydrogen-selective membrane.
52. The device of claim 51, wherein the at least one hydrogen-selective membrane is formed upon the support.
53. The device of any one of claims 51 and 52, wherein the support is adapted to support the permeate surface of the at least one hydrogen-selective membrane.
54. The device of any one of claims 51 and 53, wherein the support physically contacts and extends generally along the permeate surface of the at least one hydrogen-selective membrane.
55. The device of any one of claims 53 and 54, wherein the support engages, but is not bonded to, the permeate surface of the at least one hydrogen-selective membrane.
56. The device of any one of claims 51-55, wherein the support is formed from a porous material.
57. The device of any one of claims 51-56 wherein the support includes at least one mesh screen.
58. The device of any one of claims 43-57, wherein the at least one hydrogen-selective membrane is mounted on a frame that is housed within the enclosure.
59. The device of any one of claims 51-58, wherein the support includes a coating that is thermodynamically stable with respect to decomposition in the presence of hydrogen and which is adapted to prevent intermetallic diffusion between the support and the membrane.
60. The device of any one of claims 43-59, wherein the enclosure includes a plurality of the hydrogen-selective membranes.
61. The device of any one of claims 43-60, wherein the device includes at least one membrane envelope formed from a pair of the hydrogen-selective membranes oriented such that the pair of hydrogen-selective membranes are spaced-apart from each other with their permeate surfaces generally facing each other to define a harvesting conduit extending therebetween, and further wherein the permeate stream is formed from the portion of the mixed gas stream that passes through the membranes to the harvesting conduit, with the remaining portion of the mixed gas stream which remains on the first surface of the membranes forming at least a portion of the byproduct stream.
62. The device of claim 61, wherein the at least one membrane envelope includes a support within the harvesting conduit and adapted to support the pair of hydrogen-selective membranes, 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 pair of hydrogen-selective membranes.
63. The device of any one of claims 61 and 62, wherein the enclosure includes a plurality of membrane envelopes.
64. The device of claim 63, wherein the hydrogen purification device includes a plurality of gas transport conduits interconnecting the plurality of membrane envelopes to selectively deliver the mixed gas stream to the first surfaces of the membranes, remove the permeate stream from the harvesting conduit, and remove the byproduct stream.
65. The device of any one of claims 43-64, in combination with a fuel cell stack adapted to receive at least a portion of the permeate stream.
66. The device of any one of claims 43-65, in combination with a fuel processor having at least one hydrogen-producing region adapted to produce the mixed gas stream.
67. The device of claim 66, wherein the fuel processor is adapted to produce the mixed gas stream by steam reforming a feed stream containing water and at least one carbon-containing feedstock.
68. The device of claim 67, in further combination with a polishing assembly adapted reduce the concentration of any carbon monoxide present in the permeate stream.
69. In a hydrogen purification device that is adapted to be operated at a temperature of at least 200° C and a pressure of at least 50 psi and which includes an enclosure with an internal, at least substantially fluid-tight compartment having at least one inlet, at least one outlet, and containing at least one hydrogen-selective metal membrane adapted to separate a mixed gas stream containing hydrogen gas and other gases into a hydrogen-rich stream containing at
70 least substantially hydrogen gas and a byproduct stream containing at least a substantial portion of the other gases, the improvement comprising: the membrane being at least substantially comprised of an alloy of palladium, copper and silicon, with the silicon being present in the alloy in a concentration of no more than ppm.
70. The device of claim 69, wherein the alloy comprises no more than 15 ppm silicon.
70. The device of claim 69, wherein the alloy comprises no more than 15 ppm silicon.
71. The device of any one of claims 69 and 70, wherein the alloy further comprises carbon, with the carbon being present in the alloy in a concentration of no more than 146 ppm.
72. The device of claim 71, wherein the alloy further comprises carbon, with the carbon being present in the alloy in a concentration of no more than 56 ppm.
73. The device of any one of claims 69-72, wherein the alloy comprises approximately 40 wt% copper.
74. The device of any one of claims 69-73, wherein the alloy includes at least one additional component other than palladium, copper and oxygen.
75. The device of any one of claims 69-74, wherein the membrane includes at least one component in addition to the alloy.
76. The device of any one of claims 69-75, in combination with a fuel processor that is adapted to produce the mixed gas stream.
77. The device of any one of claims 69-76, in further combination with a fuel cell stack adapted to receive at least a portion of the hydrogen-rich stream.
Applications Claiming Priority (3)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| US08/951,091 US5997594A (en) | 1996-10-30 | 1997-10-15 | Steam reformer with internal hydrogen purification |
| US08/951,091 | 1997-10-15 | ||
| CA002427464A CA2427464C (en) | 1997-10-15 | 1998-10-14 | Steam reformer with internal hydrogen purification |
Related Parent Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CA002427464A Division CA2427464C (en) | 1997-10-15 | 1998-10-14 | Steam reformer with internal hydrogen purification |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CA2458314A1 true CA2458314A1 (en) | 1999-04-22 |
| CA2458314C CA2458314C (en) | 2011-01-04 |
Family
ID=32471136
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CA2458314A Expired - Lifetime CA2458314C (en) | 1997-10-15 | 1998-10-14 | Steam reformer with internal hydrogen purification |
Country Status (1)
| Country | Link |
|---|---|
| CA (1) | CA2458314C (en) |
Cited By (12)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107585740A (en) * | 2016-07-07 | 2018-01-16 | 乔治·克劳德方法的研究开发空气股份有限公司 | Anticorrosion reformer tubes with internal heat exchange |
| CN110844884A (en) * | 2019-10-28 | 2020-02-28 | 中科液态阳光(苏州)氢能科技发展有限公司 | Methanol steam reforming and hydrogen separation integrated device |
| US11322766B2 (en) | 2020-05-28 | 2022-05-03 | Saudi Arabian Oil Company | Direct hydrocarbon metal supported solid oxide fuel cell |
| US11492255B2 (en) | 2020-04-03 | 2022-11-08 | Saudi Arabian Oil Company | Steam methane reforming with steam regeneration |
| US11492254B2 (en) | 2020-06-18 | 2022-11-08 | Saudi Arabian Oil Company | Hydrogen production with membrane reformer |
| US11578016B1 (en) | 2021-08-12 | 2023-02-14 | Saudi Arabian Oil Company | Olefin production via dry reforming and olefin synthesis in a vessel |
| US11583824B2 (en) | 2020-06-18 | 2023-02-21 | Saudi Arabian Oil Company | Hydrogen production with membrane reformer |
| US11617981B1 (en) | 2022-01-03 | 2023-04-04 | Saudi Arabian Oil Company | Method for capturing CO2 with assisted vapor compression |
| US11639290B2 (en) | 2020-06-04 | 2023-05-02 | Saudi Arabian Oil Company | Dry reforming of methane with carbon dioxide at elevated pressure |
| US11718575B2 (en) | 2021-08-12 | 2023-08-08 | Saudi Arabian Oil Company | Methanol production via dry reforming and methanol synthesis in a vessel |
| US11787759B2 (en) | 2021-08-12 | 2023-10-17 | Saudi Arabian Oil Company | Dimethyl ether production via dry reforming and dimethyl ether synthesis in a vessel |
| US11999619B2 (en) | 2020-06-18 | 2024-06-04 | Saudi Arabian Oil Company | Hydrogen production with membrane reactor |
-
1998
- 1998-10-14 CA CA2458314A patent/CA2458314C/en not_active Expired - Lifetime
Cited By (13)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107585740B (en) * | 2016-07-07 | 2022-12-20 | 乔治·克劳德方法的研究开发空气股份有限公司 | Corrosion resistant reformer tubes with internal heat exchange |
| CN107585740A (en) * | 2016-07-07 | 2018-01-16 | 乔治·克劳德方法的研究开发空气股份有限公司 | Anticorrosion reformer tubes with internal heat exchange |
| CN110844884A (en) * | 2019-10-28 | 2020-02-28 | 中科液态阳光(苏州)氢能科技发展有限公司 | Methanol steam reforming and hydrogen separation integrated device |
| US11492255B2 (en) | 2020-04-03 | 2022-11-08 | Saudi Arabian Oil Company | Steam methane reforming with steam regeneration |
| US11322766B2 (en) | 2020-05-28 | 2022-05-03 | Saudi Arabian Oil Company | Direct hydrocarbon metal supported solid oxide fuel cell |
| US11639290B2 (en) | 2020-06-04 | 2023-05-02 | Saudi Arabian Oil Company | Dry reforming of methane with carbon dioxide at elevated pressure |
| US11583824B2 (en) | 2020-06-18 | 2023-02-21 | Saudi Arabian Oil Company | Hydrogen production with membrane reformer |
| US11492254B2 (en) | 2020-06-18 | 2022-11-08 | Saudi Arabian Oil Company | Hydrogen production with membrane reformer |
| US11999619B2 (en) | 2020-06-18 | 2024-06-04 | Saudi Arabian Oil Company | Hydrogen production with membrane reactor |
| US11578016B1 (en) | 2021-08-12 | 2023-02-14 | Saudi Arabian Oil Company | Olefin production via dry reforming and olefin synthesis in a vessel |
| US11718575B2 (en) | 2021-08-12 | 2023-08-08 | Saudi Arabian Oil Company | Methanol production via dry reforming and methanol synthesis in a vessel |
| US11787759B2 (en) | 2021-08-12 | 2023-10-17 | Saudi Arabian Oil Company | Dimethyl ether production via dry reforming and dimethyl ether synthesis in a vessel |
| US11617981B1 (en) | 2022-01-03 | 2023-04-04 | Saudi Arabian Oil Company | Method for capturing CO2 with assisted vapor compression |
Also Published As
| Publication number | Publication date |
|---|---|
| CA2458314C (en) | 2011-01-04 |
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| EEER | Examination request | ||
| MKEX | Expiry |
Effective date: 20181015 |