JP4255941B2 - 酸素透過膜を用いた炭化水素改質方法及び炭化水素改質装置 - Google Patents
酸素透過膜を用いた炭化水素改質方法及び炭化水素改質装置 Download PDFInfo
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- JP4255941B2 JP4255941B2 JP2005303915A JP2005303915A JP4255941B2 JP 4255941 B2 JP4255941 B2 JP 4255941B2 JP 2005303915 A JP2005303915 A JP 2005303915A JP 2005303915 A JP2005303915 A JP 2005303915A JP 4255941 B2 JP4255941 B2 JP 4255941B2
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- 239000001301 oxygen Substances 0.000 title claims description 96
- 229910052760 oxygen Inorganic materials 0.000 title claims description 96
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 title claims description 94
- 239000012528 membrane Substances 0.000 title claims description 85
- 238000002407 reforming Methods 0.000 title claims description 42
- 239000004215 Carbon black (E152) Substances 0.000 title claims description 28
- 229930195733 hydrocarbon Natural products 0.000 title claims description 28
- 150000002430 hydrocarbons Chemical class 0.000 title claims description 27
- 238000000034 method Methods 0.000 title description 20
- 239000007789 gas Substances 0.000 claims description 69
- 238000006243 chemical reaction Methods 0.000 claims description 50
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 21
- 229910000420 cerium oxide Inorganic materials 0.000 claims description 5
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 claims description 5
- 229910052596 spinel Inorganic materials 0.000 claims description 5
- 239000011029 spinel Substances 0.000 claims description 5
- 125000001183 hydrocarbyl group Chemical group 0.000 claims 1
- 238000007254 oxidation reaction Methods 0.000 description 43
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 36
- 229910052739 hydrogen Inorganic materials 0.000 description 33
- 239000001257 hydrogen Substances 0.000 description 32
- 230000003647 oxidation Effects 0.000 description 31
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 27
- 239000010408 film Substances 0.000 description 26
- 238000000629 steam reforming Methods 0.000 description 25
- 238000006057 reforming reaction Methods 0.000 description 21
- 230000008859 change Effects 0.000 description 13
- 238000001816 cooling Methods 0.000 description 9
- 230000015572 biosynthetic process Effects 0.000 description 8
- 238000003786 synthesis reaction Methods 0.000 description 8
- 238000004519 manufacturing process Methods 0.000 description 7
- 229910002091 carbon monoxide Inorganic materials 0.000 description 6
- 238000010586 diagram Methods 0.000 description 6
- 238000000926 separation method Methods 0.000 description 6
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 5
- 230000005540 biological transmission Effects 0.000 description 5
- 150000002431 hydrogen Chemical class 0.000 description 5
- 238000013021 overheating Methods 0.000 description 5
- 230000008569 process Effects 0.000 description 5
- 239000002994 raw material Substances 0.000 description 5
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 4
- 239000000446 fuel Substances 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- 239000000203 mixture Substances 0.000 description 4
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- -1 oxygen ion Chemical class 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 2
- ATUOYWHBWRKTHZ-UHFFFAOYSA-N Propane Chemical compound CCC ATUOYWHBWRKTHZ-UHFFFAOYSA-N 0.000 description 2
- 229910002092 carbon dioxide Inorganic materials 0.000 description 2
- 239000001569 carbon dioxide Substances 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 150000002500 ions Chemical class 0.000 description 2
- 238000005259 measurement Methods 0.000 description 2
- 239000010409 thin film Substances 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 description 1
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 238000002453 autothermal reforming Methods 0.000 description 1
- 239000001273 butane Substances 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 238000004891 communication Methods 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 239000004020 conductor Substances 0.000 description 1
- 230000006378 damage Effects 0.000 description 1
- 230000002950 deficient Effects 0.000 description 1
- 230000000593 degrading effect Effects 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000000605 extraction Methods 0.000 description 1
- 239000003502 gasoline Substances 0.000 description 1
- 230000012447 hatching Effects 0.000 description 1
- 230000020169 heat generation Effects 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 230000037427 ion transport Effects 0.000 description 1
- 239000003350 kerosene Substances 0.000 description 1
- 238000010030 laminating Methods 0.000 description 1
- 238000003475 lamination Methods 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 239000011533 mixed conductor Substances 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- IJDNQMDRQITEOD-UHFFFAOYSA-N n-butane Chemical compound CCCC IJDNQMDRQITEOD-UHFFFAOYSA-N 0.000 description 1
- OFBQJSOFQDEBGM-UHFFFAOYSA-N n-pentane Natural products CCCCC OFBQJSOFQDEBGM-UHFFFAOYSA-N 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- 230000035699 permeability Effects 0.000 description 1
- 230000008092 positive effect Effects 0.000 description 1
- 239000001294 propane Substances 0.000 description 1
- 239000012495 reaction gas Substances 0.000 description 1
- 229920006395 saturated elastomer Polymers 0.000 description 1
- 238000003746 solid phase reaction Methods 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- 238000006557 surface reaction Methods 0.000 description 1
- 238000010345 tape casting Methods 0.000 description 1
- 238000012932 thermodynamic analysis Methods 0.000 description 1
- 230000032258 transport Effects 0.000 description 1
Images
Classifications
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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
- B01D63/08—Flat membrane modules
- B01D63/082—Flat membrane modules comprising a stack of flat membranes
-
- 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
- B01D63/08—Flat membrane modules
- B01D63/082—Flat membrane modules comprising a stack of flat membranes
- B01D63/0822—Plate-and-frame devices
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B13/00—Oxygen; Ozone; Oxides or hydroxides in general
- C01B13/02—Preparation of oxygen
- C01B13/0229—Purification or separation processes
- C01B13/0248—Physical processing only
- C01B13/0251—Physical processing only by making use of membranes
-
- 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
- C01B3/386—Catalytic partial combustion
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/10—Single element gases other than halogens
- B01D2257/104—Oxygen
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2311/00—Details relating to membrane separation process operations and control
- B01D2311/10—Temperature control
-
- 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
- C01B2203/025—Processes for making hydrogen or synthesis gas containing a partial oxidation step
- C01B2203/0261—Processes for making hydrogen or synthesis gas containing a partial oxidation step containing a catalytic partial oxidation step [CPO]
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2210/00—Purification or separation of specific gases
- C01B2210/0043—Impurity removed
- C01B2210/0046—Nitrogen
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2210/00—Purification or separation of specific gases
- C01B2210/0043—Impurity removed
- C01B2210/0053—Hydrogen
Description
(1)+(4) CH4+2H2O→CO2+4H2 ΔH=190.9
kJ/mol (吸熱) 式(6)
のような反応が用いられる。これらは上から順に、水蒸気改質、オートサーマル改質、部分酸化改質と呼ばれる。また、合成ガスを得る場合にも、
のように、水蒸気と酸素を併用するオートサーマル法がよく用いられる。
さらに望ましい対応露点温度は、70℃乃至80℃である(4)。
[CO], [CO2], [H2], [H2O])から各々以下の式で計算された。
比から反応器内で起こった部分酸化改質反応と水蒸気改質反応の比率を推定することが可能であり、試料7の場合、製造された水素は76%が部分酸化改質由来、24%程度が水蒸気改質由来であると計算された。また、本発明による酸素透過膜の冷却効果については、40℃加湿の試験、例えば表2の試料1,2等はメタン投入後数10分で膜が破壊したが、80℃加湿のその他の試料ではそのような膜の破壊は確認されなかったことから確認された。
Wであり、実際の発熱量17.46 Wよりも大きく冷却能に余裕があることが伺える。よって、本発明が提供する水蒸気改質による酸素透過膜の冷却は有効に機能していると言える。
2A、2B 平板ユニット
2C 蓋板ユニット
2D 底板ユニット
3a 原料ガス流入部
3b 改質ガス流出部
4a 空気流入部
4b 空気流出部
11a、11b、12a、12b マニホールド孔部
15 酸素透過膜
16 ボルト貫通孔
17 フランジ部
18 膜保持部
19 ガス流路用溝部
Claims (4)
- 直交する二つの中心軸に対してそれぞれ対称形状の平板ユニットを90度回転させた平板ユニット対を交互に積層し、蓋板ユニットと底板ユニットとで挟んで成るスタック構造改質装置であって、
各平板ユニットは、中央部に反応室用孔部を有する膜保持部と、
膜保持部に固定された特定ガス透過膜と、
膜保持部を囲み、かつ、膜保持部より一段高く形成されたフランジ部と、
フランジ部には、第一の中心軸上に、膜保持部を挟んで設けられた第一のガス流入用マニホールド孔部及びガス流出用マニホールド孔部と、
第一の中心軸と直交する第二の中心軸上に、膜保持部を挟んで設けられた第二のガス流入用マニホールド孔部及びガス流出用マニホールド孔部と、
第一のガス流入用マニホールド孔部及びガス流出用マニホールド孔部と、膜保持部とを連通させるガス流路部と、
を備えて成ることを特徴とする改質装置。 - 前記改質装置が炭化水素改質装置であり、前記特定ガス透過膜が酸素透過膜であり、かつ、第一のガス流入用マニホールド孔部には炭化水素ガス及び水蒸気を、第二のガス流入用マニホールド孔部には空気を、流入するように構成して成ることを特徴とする請求項1に記載の改質装置。
- 前記酸素透過膜が、セリウム酸化物とスピネル型酸化物から構成される複合体型酸素透過膜であることを特徴とする請求項1又は2に記載の改質装置。
- 前記酸素透過膜の膜厚が、100μm乃至1cmであることを特徴とする請求項1乃至3に記載の改質装置。
Priority Applications (4)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
JP2005303915A JP4255941B2 (ja) | 2005-10-19 | 2005-10-19 | 酸素透過膜を用いた炭化水素改質方法及び炭化水素改質装置 |
PCT/JP2006/320532 WO2007046314A1 (ja) | 2005-10-19 | 2006-10-16 | 酸素透過膜を用いた炭化水素改質方法及び炭化水素改質装置 |
US11/992,894 US7922780B2 (en) | 2005-10-19 | 2006-10-16 | Method and apparatus for hydrocarbon reforming based on oxygen-permeable membrane |
EP06811803A EP2045212B1 (en) | 2005-10-19 | 2006-10-16 | Hydrogen reforming method and hydrogen reforming device using oxygen-permeable membrane |
Applications Claiming Priority (1)
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JP2005303915A JP4255941B2 (ja) | 2005-10-19 | 2005-10-19 | 酸素透過膜を用いた炭化水素改質方法及び炭化水素改質装置 |
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JP2007112646A JP2007112646A (ja) | 2007-05-10 |
JP4255941B2 true JP4255941B2 (ja) | 2009-04-22 |
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Country Status (4)
Country | Link |
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US (1) | US7922780B2 (ja) |
EP (1) | EP2045212B1 (ja) |
JP (1) | JP4255941B2 (ja) |
WO (1) | WO2007046314A1 (ja) |
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US9340297B2 (en) * | 2013-02-19 | 2016-05-17 | The Boeing Company | Counter-flow gas separation modules and methods |
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US9611144B2 (en) | 2013-04-26 | 2017-04-04 | Praxair Technology, Inc. | Method and system for producing a synthesis gas in an oxygen transport membrane based reforming system that is free of metal dusting corrosion |
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EP3055052A2 (en) * | 2013-10-07 | 2016-08-17 | Praxair Technology Inc. | Ceramic oxygen transport membrane array reactor and reforming method |
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CN105764842B (zh) | 2013-12-02 | 2018-06-05 | 普莱克斯技术有限公司 | 使用具有二段转化的基于氧转运膜的重整系统生产氢气的方法和系统 |
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JP2007112646A (ja) | 2007-05-10 |
EP2045212A1 (en) | 2009-04-08 |
WO2007046314A1 (ja) | 2007-04-26 |
EP2045212B1 (en) | 2011-08-24 |
US7922780B2 (en) | 2011-04-12 |
EP2045212A4 (en) | 2010-03-24 |
US20100178238A1 (en) | 2010-07-15 |
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