JP4180380B2 - 水素および窒素含有ガス混合物の製造方法 - Google Patents
水素および窒素含有ガス混合物の製造方法 Download PDFInfo
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- JP4180380B2 JP4180380B2 JP2002571397A JP2002571397A JP4180380B2 JP 4180380 B2 JP4180380 B2 JP 4180380B2 JP 2002571397 A JP2002571397 A JP 2002571397A JP 2002571397 A JP2002571397 A JP 2002571397A JP 4180380 B2 JP4180380 B2 JP 4180380B2
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- Prior art keywords
- hydrogen
- gas
- membrane
- synthesis gas
- nitrogen
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- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 200
- 239000001257 hydrogen Substances 0.000 title claims abstract description 195
- 239000007789 gas Substances 0.000 title claims abstract description 184
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 121
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 title claims abstract description 52
- 239000000203 mixture Substances 0.000 title claims abstract description 45
- 229910052757 nitrogen Inorganic materials 0.000 title claims abstract description 26
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 21
- 239000012528 membrane Substances 0.000 claims abstract description 135
- 238000000034 method Methods 0.000 claims abstract description 80
- 150000002431 hydrogen Chemical class 0.000 claims abstract description 74
- 230000015572 biosynthetic process Effects 0.000 claims abstract description 61
- 238000003786 synthesis reaction Methods 0.000 claims abstract description 59
- 239000012466 permeate Substances 0.000 claims abstract description 51
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 44
- 239000001301 oxygen Substances 0.000 claims abstract description 44
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 41
- 230000003197 catalytic effect Effects 0.000 claims abstract description 16
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 claims abstract description 16
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 9
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 9
- 239000000376 reactant Substances 0.000 claims abstract description 7
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 43
- 238000006243 chemical reaction Methods 0.000 claims description 20
- 239000000446 fuel Substances 0.000 claims description 11
- 238000000629 steam reforming Methods 0.000 claims description 11
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 8
- 238000002485 combustion reaction Methods 0.000 claims description 7
- 229910021529 ammonia Inorganic materials 0.000 claims description 4
- 239000012465 retentate Substances 0.000 abstract description 7
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 38
- 238000000926 separation method Methods 0.000 description 17
- 239000003345 natural gas Substances 0.000 description 11
- 239000003054 catalyst Substances 0.000 description 10
- 239000007800 oxidant agent Substances 0.000 description 8
- 239000000047 product Substances 0.000 description 8
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 7
- 230000001590 oxidative effect Effects 0.000 description 7
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 6
- 229910002091 carbon monoxide Inorganic materials 0.000 description 6
- 238000005265 energy consumption Methods 0.000 description 5
- 230000003647 oxidation Effects 0.000 description 5
- 238000007254 oxidation reaction Methods 0.000 description 5
- 238000010248 power generation Methods 0.000 description 5
- 229910021536 Zeolite Inorganic materials 0.000 description 4
- 239000000567 combustion gas Substances 0.000 description 4
- 150000001875 compounds Chemical class 0.000 description 4
- 238000001816 cooling Methods 0.000 description 4
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 4
- 239000010408 film Substances 0.000 description 4
- 230000020169 heat generation Effects 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- -1 oxygen ions Chemical class 0.000 description 4
- 238000011084 recovery Methods 0.000 description 4
- 239000010457 zeolite Substances 0.000 description 4
- 229910052751 metal Inorganic materials 0.000 description 3
- 239000002184 metal Substances 0.000 description 3
- 239000011148 porous material Substances 0.000 description 3
- 238000011144 upstream manufacturing Methods 0.000 description 3
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 2
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 2
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 2
- 238000009833 condensation Methods 0.000 description 2
- 230000005494 condensation Effects 0.000 description 2
- 230000005684 electric field Effects 0.000 description 2
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- 229910001252 Pd alloy Inorganic materials 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- 229910010413 TiO 2 Inorganic materials 0.000 description 1
- 229910052783 alkali metal Inorganic materials 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 239000002826 coolant Substances 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 239000003085 diluting agent Substances 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000003546 flue gas Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000010408 sweeping Methods 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
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- Hydrogen, Water And Hydrids (AREA)
- Separation Using Semi-Permeable Membranes (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
- Low-Molecular Organic Synthesis Reactions Using Catalysts (AREA)
- Food Preservation Except Freezing, Refrigeration, And Drying (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Description
(1)CH4 + H2O = CO + 3H2
水蒸気と炭素の比が一般に2〜4の間であるように、水蒸気が添加される。
(2) CO + H2O = CO2 +H2
熱は通常、水蒸気の生成により回収される。
(3) CH4 + 0.5O2 = CO + H2
ゼオライト膜は、支持体(例えば、g−Al2O3上に堆積させたシリカライト−1)の表面上または孔構造中に、ゼオライト結晶を形成することにより調製され得る。
多孔質膜およびゼオライト膜は、水素に対して100%選択性ではなく、他の化合物は膜を透過し、100%未満の水素を有する生成物を与えるであろう。
本発明の別の目的は、低減されたエネルギー消費および投資コストを伴うやり方で、水素および窒素含有ガス混合物を製造することであった。
さらに、本発明の別の目的は、低減されたエネルギー消費および投資コストを伴うやり方で、触媒または非触媒プロセスを実施する方法に到達することであった。
窒素含有スイープガス流を生成する様々な方法を評価した後、本発明者等は、水素輸送用膜を適用する実現性をさらに研究することにした。
水素輸送膜ユニットは、水素透過性膜により分けられた未透過物側および透過物側を含む装置である。
水素輸送膜反応器は、水素透過性膜により分けられた未透過物側および透過物側を含む装置であり、ここでは未透過物側には、H2Oを用いてCOをCO2とH2に変換することが可能であり、またH2Oを用いてCH4をCOとH2に変換することが可能な触媒を配備している。
下流のユニットが水素輸送膜反応器である場合、膜反応器の未透過物側に入った合成ガス中の水素の大部分と、膜反応器の未透過水側で生成したさらなる水素の大部分とが、膜反応器の透過物側に輸送され、さらに上流の発生器で生成した窒素および水蒸気含有スイープガスにより獲得される。
続いて、スイープガスおよび水素の生成混合物は、触媒または非触媒プロセスの反応物として、例えばガスタービン燃焼器における燃料として、あるいはアンモニア生産用の合成ガスの生産における反応物として利用される。
本発明は、実施例および相当する図面においてさらに説明および考察される。
あるいは、空気侵入用ユニット39は、分離型圧縮機で圧縮されてもよい。
Claims (8)
- 水素および窒素含有ガス混合物を製造する方法であって、
水蒸気および炭素含有ガスの混合物が、少なくとも1つの水素輸送膜型合成ガスおよびスイープガス発生器の未透過物側に供給され、該ガス発生器において、前記ガスおよび水蒸気は合成ガスに変換される工程と、
前記合成ガス中の水素の一部は、該水素輸送膜を通って、前記発生器中の透過物側へ輸送され、そこで、該水素の一部は、前記透過物側へ供給された空気流中の酸素と反応して、熱ならびに窒素および水蒸気含有ガスを生成する工程と、
該合成ガスは、下流水素輸送膜ユニットまたは水素輸送膜反応器の未透過物側にさらに供給され、そこで、前記合成ガス中の水素の主要部分、および反応器が使用される場合には前記反応器中の未透過物側で生成したさらなる水素の主要部分は、前記下流膜を通って輸送され、前記窒素含有ガスにより獲得されて、水素および窒素含有ガス混合物を形成する工程と、
を含むことを特徴とする方法。 - 発生した熱は、前記空気流および前記発生器に供給される他のガスを加熱するのに部分的に使用され、前記炭素含有供給ガスの水蒸気改質のための熱要件を満たすために前記発生器の前記未透過物側へ部分的に逆移動されることを特徴とする、請求項1に記載の方法。
- 前記水素輸送膜ユニットまたは前記水素輸送膜反応器を出た水素枯渇合成ガス流中の可燃性成分は、混合伝導膜反応器の未透過物側にある膜表面上で直接CO2および水に酸化されることを特徴とする、請求項1に記載の方法。
- 前記水素輸送膜ユニットまたは前記水素輸送膜反応器を出た水素枯渇合成ガス流中の可燃性成分は、混合伝導膜を用いてあるいは他のプロセスのいずれかを用いて、空気から分離される酸素と反応して、CO2および水を生成することを特徴とする、請求項1に記載の方法。
- 水素枯渇合成ガスの燃焼により発生した熱は、ガスタービン燃焼器に供給される空気を予熱するのに使用されることを特徴とする、請求項3または4に記載の方法。
- 触媒または非触媒プロセスを実施する方法であって、請求項1ないし5に記載の方法により製造される前記水素および窒素含有ガス混合物は、前記プロセスにおける反応物の1つとして適用されることを特徴とする方法。
- 前記プロセスは、アンモニア生産のためのプロセスであることを特徴とする、請求項6に記載の方法。
- 前記プロセスは燃焼プロセスであり、前記水素および窒素含有ガス混合物は、燃料として適用されることを特徴とする、請求項7に記載の方法。
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NO20010784A NO317382B1 (no) | 2001-02-16 | 2001-02-16 | Metode for a utfore en katalytisk eller ikke-katalytisk prosess |
PCT/NO2002/000058 WO2002072470A1 (en) | 2001-02-16 | 2002-02-11 | Method for manufacturing a hydrogen and nitrogen containing gas mixture |
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US (1) | US7163648B2 (ja) |
EP (1) | EP1370485B1 (ja) |
JP (1) | JP4180380B2 (ja) |
AT (1) | ATE275528T1 (ja) |
CA (1) | CA2438589C (ja) |
DE (1) | DE60201179T2 (ja) |
DK (1) | DK1370485T3 (ja) |
ES (1) | ES2227422T3 (ja) |
NO (1) | NO317382B1 (ja) |
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DE102004049076A1 (de) * | 2004-10-08 | 2006-04-13 | Uhde Gmbh | Verfahren zur Erzeugung von Synthesegas für eine Ammoniakanlage |
NO20051895D0 (no) | 2005-04-19 | 2005-04-19 | Statoil Asa | Fremgangsmate for produksjon av elektrisk energi og CO2 fra et hydrokarbon rastoff |
NO20051891D0 (no) * | 2005-04-19 | 2005-04-19 | Statoil Asa | Prosess for produksjon av elektrisk energi og CO2 fra et hydrokarbon rastoff |
US7909898B2 (en) * | 2006-02-01 | 2011-03-22 | Air Products And Chemicals, Inc. | Method of treating a gaseous mixture comprising hydrogen and carbon dioxide |
WO2008127745A2 (en) * | 2007-01-10 | 2008-10-23 | Praxair Technology, Inc. | Asu nitrogen sweep gas in hydrogen separation membrane for production of hrsg duct burner fuel |
US20080311022A1 (en) * | 2007-06-14 | 2008-12-18 | Battelle Energy Alliance, Llc | Methods and apparatuses for ammonia production |
US8495882B2 (en) * | 2009-08-10 | 2013-07-30 | General Electric Company | Syngas cleanup section with carbon capture and hydrogen-selective membrane |
US20120102964A1 (en) * | 2010-10-29 | 2012-05-03 | General Electric Company | Turbomachine including a carbon dioxide (co2) concentration control system and method |
DE102012212708A1 (de) * | 2012-07-19 | 2014-01-23 | Thyssenkrupp Marine Systems Gmbh | Verfahren zum Abscheiden von Wasserstoff aus einem wasserstoffhaltigen Gasgemisch und Vorrichtung zur Durchführung dieses Verfahrens |
TWI495510B (zh) * | 2013-10-29 | 2015-08-11 | Atomic Energy Council | Fibrous membrane reaction device |
JP6702884B2 (ja) * | 2014-12-26 | 2020-06-03 | 日本碍子株式会社 | ガス分離方法 |
JP6636948B2 (ja) * | 2014-12-26 | 2020-01-29 | 日本碍子株式会社 | ガス分離方法 |
US11994063B2 (en) * | 2019-10-16 | 2024-05-28 | Richard Alan Callahan | Turbine powered electricity generation |
US11654401B2 (en) * | 2021-10-25 | 2023-05-23 | Generon Igs, Inc. | Gas separation membrane cartridge with clamshell retainer |
US11808206B2 (en) | 2022-02-24 | 2023-11-07 | Richard Alan Callahan | Tail gas recycle combined cycle power plant |
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US3901668A (en) * | 1973-11-05 | 1975-08-26 | Sun Ventures Inc | Manufacture of oxygen from high temperature steam |
SU798031A1 (ru) | 1975-04-07 | 1981-01-23 | Предприятие П/Я Р-6603 | Способ получени аммиака и метанола |
US4172885A (en) * | 1978-03-20 | 1979-10-30 | Monsanto Company | Process for the recovery of hydrogen from ammonia purge gases |
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CA2438589C (en) | 2010-05-25 |
CA2438589A1 (en) | 2002-09-19 |
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EP1370485B1 (en) | 2004-09-08 |
NO20010784D0 (no) | 2001-02-16 |
DE60201179D1 (de) | 2004-10-14 |
ATE275528T1 (de) | 2004-09-15 |
DK1370485T3 (da) | 2005-01-24 |
US7163648B2 (en) | 2007-01-16 |
EP1370485A1 (en) | 2003-12-17 |
PT1370485E (pt) | 2005-01-31 |
ES2227422T3 (es) | 2005-04-01 |
WO2002072470A1 (en) | 2002-09-19 |
US20040170557A1 (en) | 2004-09-02 |
DE60201179T2 (de) | 2005-10-13 |
NO20010784L (no) | 2002-08-19 |
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