JP2008526676A - 水素ガス流から一酸化炭素を除去する装置及び方法 - Google Patents
水素ガス流から一酸化炭素を除去する装置及び方法 Download PDFInfo
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- JP2008526676A JP2008526676A JP2007549901A JP2007549901A JP2008526676A JP 2008526676 A JP2008526676 A JP 2008526676A JP 2007549901 A JP2007549901 A JP 2007549901A JP 2007549901 A JP2007549901 A JP 2007549901A JP 2008526676 A JP2008526676 A JP 2008526676A
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- catalyst
- carbon monoxide
- gas
- gas stream
- reactor
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- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 title claims abstract description 61
- 229910002091 carbon monoxide Inorganic materials 0.000 title claims abstract description 61
- 238000000034 method Methods 0.000 title claims abstract description 48
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 37
- 239000003054 catalyst Substances 0.000 claims abstract description 96
- 239000007789 gas Substances 0.000 claims abstract description 87
- 239000001257 hydrogen Substances 0.000 claims abstract description 32
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 32
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims abstract description 32
- 239000000463 material Substances 0.000 claims abstract description 29
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 13
- 239000002638 heterogeneous catalyst Substances 0.000 claims abstract description 5
- 238000005984 hydrogenation reaction Methods 0.000 claims description 38
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- 238000012856 packing Methods 0.000 claims description 32
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- 125000003118 aryl group Chemical group 0.000 claims description 3
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- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
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Classifications
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- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
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- C01B3/586—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids including a catalytic reaction the reaction being a methanation reaction
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- B01J37/34—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation
- B01J37/341—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 electric or magnetic fields, wave energy or particle radiation
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- C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
- C01B2203/0435—Catalytic purification
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Abstract
【解決手段】不均一系触媒の存在下で、一酸化炭素を水素と反応させてメタン及び水を生じさせることによって、水素ガス流から一酸化炭素を除去する方法であって、
前記触媒が、担体材料上に薄層触媒として存在することを特徴とする方法。
【選択図】なし
Description
900℃で前焼成して織られたカンタル(Kanthal)織物に、硝酸ニトロシルRu塩溶液を含浸させた後、120℃で1時間乾燥させた。含浸のため、20.3質量%のRu(NO)(NO3)3水溶液を蒸留水で0.7質量%のRuまで希釈した。含浸は、金属製の織物リボンを含浸液で満たされた平皿から引き出す手動の含浸装置において行った。これは、金属製織物をRu含有含浸液で湿らせた。その後、まだ湿っている濡れた金属製の織物リボンをIRラジエータを用いて乾燥域中で予備乾燥させ、次に、周囲空気の存在下、乾燥オーブン中、120℃で乾燥させた。乾燥時間は1時間であった。乾燥後、IR−含浸カンタル織物を巻いて、構造化織物パッキングを形成した。完成したRu−飽和カンタル織物を、4時間、メタン化反応器中、120℃でH2雰囲気下、周囲圧力で還元した。ルテニウムを含んでいる表面は、580mgRu/カンタル織物m2に相当する。
実施例1により製造されたRu/カンタル触媒を、周囲圧力、CO含有水素流でチャージされたオイル加熱ジャケット付管においてテストした。反応器下流のオフガス流中の残留CO濃度を、Uras製CO分析器を用いて測定した。メタン化実験において一酸化炭素の完全分解が観察された際の温度及びCO濃度の関数として、最大触媒空間速度を表1に示す。第1カラムにおいて、メタン化が実施された温度を記録した。第2カラムは、COが25ppmの出発濃度で完全に分解した際のGHSV(ガス時間空間速度)を示す。第3カラムでは、100ppmの出発濃度でCOが完全に分解した際のGHSVを記録した。これにより、180℃の反応器温度及び3053h-1のGHSVで、100ppmのCO濃度が7時間かけて完全に分解した。一方、80℃で、一酸化炭素の完全分解が、ほぼ325h-1の最大GHSV、25ppmの出発CO濃度で達された。
リスメラールをPd/C触媒の存在下で還流しながら沸騰させ、H2を用いて形成したガスを反応充填物から排出し、オイル加熱されたジャケット付き管中に収容されたRu−カンタル織物パッキングに通した。供給されたガスのCO導入は150〜250ppmの範囲内であった。温度は、初めの15時間内は140℃であり、さらなる実験経過では180℃であった。反応器から出たガス流の一酸化炭素分析は、供給された一酸化炭素の完全分解を示した。GHSVは2600h-1であった。
COメタン化触媒を製造するため、900℃で前焼成したRu含浸の織られた、しわがないカンタル織物からなる構造化パッキングを巻いて、9.5mmの厚い構造化織物パッキングを形成した。構造化パッキングの中央に熱電素子用の凹所がある。当該凹所の直径は、3.17mmであった。終了前に、前記織物を硝酸Ru(III)溶液で含浸させた後、乾燥させ、空気下、200℃で2時間、熱処理した。全長で、反応器は1170cm2で充填された。実際の実験の前に、製造した触媒を、メタン化反応器中で、80℃、120℃、180℃、及び200℃で、それぞれ1時間、段階的に速やかに還元した。Ruを含んでいる表面は、2075mgRu/カンタル織物m2であった。
実施例4において製造されたRu/カンタル触媒を、既知濃度のCO含有H2流とともに2013mbaraでオイル加熱されたジャケット付き管中に装填した。反応器全体に、6個の別々の構造化パッキング(5個のパッキングがそれぞれ8cmの長さであり、1個のパッキングが5cmの長さである)を装填した。反応組成物は、燃料電池用途への炭化水素の改質に典型的なモル比で、H2及びCOに加えて、CO2、N2及びH2Oを含んでいた。表2は、反応器の上流及び下流のガス組成を示す。確定したGHSVは1800h-1であった。反応器温度は200℃であった。反応の間、構造化パッキング上でのいかなる圧力損失も測定されなかった、すなわち測定中の圧力損失は100mbar未満(測定装置の検出感度)であった。当該実験において、COをほとんど完全に分解した。
Claims (15)
- 不均一系触媒の存在下で、一酸化炭素を水素と反応させてメタン及び水を生じさせることによって、水素ガス流から一酸化炭素を除去する方法であって、
前記触媒が、担体材料上に薄層触媒として存在することを特徴とする方法。 - 担体材料が、リボン、箔、織物、又はループ線状編物の形態で存在することを特徴とする請求項1に記載の方法。
- 担体材料が、織物又は編物の形態であることを特徴とする請求項2に記載の方法。
- 編物が、構造化パッキングの形態に加工されたものであることを特徴とする請求項3に記載の方法。
- 触媒を含む担体材料の表面が、表面積m2あたり3000mg未満の触媒を含むことを特徴とする請求項1〜4のいずれか1項に記載の方法。
- 触媒が、Ru、Ni、Pt、Pd、Rh、Cu、及びこれらの混合物の元素から選択されることを特徴とする請求項1〜5のいずれか1項に記載の方法。
- 水素リッチガス流が、化学プラントからの循環ガスであることを特徴とする請求項1〜6のいずれか1項に記載の方法。
- 循環ガスが、水素化からの汚染された水素であることを特徴とする請求項7に記載の方法。
- α,β−不飽和アルデヒド又は芳香族基を有するアルデヒドを水素化することを特徴とする請求項8に記載の方法。
- 循環ガスの一部をオフガスとして周囲に排出することを特徴とする請求項7〜9のいずれか1項に記載の方法。
- 水素リッチガス流が、燃料電池用燃料として使用される請求項1〜6のいずれか1項に記載の方法。
- メタン化反応器を有する、請求項1〜11のいずれか1項に記載の方法を実施するための装置であって、
担持材料に担持された薄層触媒が、メタン化反応器内に収容されていることを特徴とする装置。 - メタン化反応器の壁が、ジャケットを設けた設計とされていることを特徴とする請求項12に記載の装置。
- 担体材料に担持された薄層触媒が、別々の構造化パッキング素子の形態に加工されていることを特徴とする請求項12又は13に記載の装置。
- 円盤状反応器充填物が、構造化パッキング素子から形成され、且つ異なる方向で交互に走行する流路を形成するように配列されることを特徴とする請求項14に記載の装置。
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DE102005001290A DE102005001290A1 (de) | 2005-01-11 | 2005-01-11 | Vorrichtung und Verfahren zur Entfernung von Kohlenmonoxid aus einem wasserstoffhaltigen Gasstrom |
PCT/EP2006/050100 WO2006074988A1 (de) | 2005-01-11 | 2006-01-09 | Vorrichtung und verfahren zur entfernung von kohlenmonoxid aus einem wasserstoffhaltigen gasstrom |
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DE102005049568A1 (de) | 2005-10-17 | 2007-04-19 | Basf Ag | Verfahren zur kontinuierlichen Hydrierung oder hydrierenden Aminierung |
DE102005055632A1 (de) * | 2005-11-22 | 2007-05-24 | Fraunhofer-Gesellschaft zur Förderung der angewandten Forschung e.V. | Verbundsystem und dessen Verwendung sowie Verfahren zum sauerstofffreien Verpacken von oxidationsempfindlichen Verpackungsgütern |
DE102008002535A1 (de) | 2007-06-25 | 2009-01-02 | Basf Se | Verfahren zur Herstellung vicinaler Dioxoverbindungen durch Oxidation vicinaler Dihydroxyverbindungen an Silber enthaltenden Dünnschichtkatalysatoren |
KR101329082B1 (ko) * | 2011-11-25 | 2013-11-14 | 한국원자력연구원 | 광섬유 레이저를 이용한 탄소 및 산소 동위원소 분리 방법 및 장치 |
JP2019531184A (ja) * | 2016-09-23 | 2019-10-31 | ビーエーエスエフ ソシエタス・ヨーロピアBasf Se | 有機化合物の水素化のための触媒活性固定床を提供する方法 |
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EP1246286A1 (de) | 2001-03-31 | 2002-10-02 | OMG AG & Co. KG | Kombinierte Kraft- Wärmeanlage mit Gaserzeugungssystem und Brennstoffzellen sowie Verfahren zu ihrem Betrieb |
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EP1435672A1 (de) * | 2002-12-30 | 2004-07-07 | Umicore AG & Co. KG | Katalysatorhaltiges Gasverteilersubstrat für Brennstoffzellen sowie Verfahren zu dessen Herstellung |
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JPS58159426A (ja) * | 1982-03-01 | 1983-09-21 | オリン・コ−ポレイシヨン | 改良されたメタン化方法 |
JPH11508817A (ja) * | 1995-07-08 | 1999-08-03 | ビーエーエスエフ アクチェンゲゼルシャフト | 物質交換塔中で使用するための規則的配列構造を有する圧力損失の少ない織物充填物又は織物類似の充填物及びこの充填物の使用下での精留方法 |
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JP2004529068A (ja) * | 2000-10-13 | 2004-09-24 | ビーエーエスエフ アクチェンゲゼルシャフト | 構造化担体または一体式担体を有する触媒を使用した非置換またはアルキル基置換の芳香族炭化水素の水素化方法 |
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