JP5890380B2 - フィッシャー・トロプシュ合成の触媒構造物及び方法 - Google Patents
フィッシャー・トロプシュ合成の触媒構造物及び方法 Download PDFInfo
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- JP5890380B2 JP5890380B2 JP2013249068A JP2013249068A JP5890380B2 JP 5890380 B2 JP5890380 B2 JP 5890380B2 JP 2013249068 A JP2013249068 A JP 2013249068A JP 2013249068 A JP2013249068 A JP 2013249068A JP 5890380 B2 JP5890380 B2 JP 5890380B2
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- 238000004519 manufacturing process Methods 0.000 claims description 11
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Classifications
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- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G2/00—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon
- C10G2/30—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen
- C10G2/32—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts
- C10G2/33—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts characterised by the catalyst used
- C10G2/331—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts characterised by the catalyst used containing group VIII-metals
- C10G2/332—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts characterised by the catalyst used containing group VIII-metals of the iron-group
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- B01J12/00—Chemical processes in general for reacting gaseous media with gaseous media; Apparatus specially adapted therefor
- B01J12/007—Chemical processes in general for reacting gaseous media with gaseous media; Apparatus specially adapted therefor in the presence of catalytically active bodies, e.g. porous plates
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- B01J23/89—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals
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Description
(A)参照
更に、本発明は: 第一細孔表面領域と、少なくとも約0.1μmの第一細孔サイズとを有する触媒構造物を提供する工程;
任意に、多孔質担体上に配置された緩衝層;
第二細孔表面領域と該第一細孔サイズ未満の第二細孔サイズとを有する多孔質界面層であって、該緩衝層(存在している場合)上に又は該第一細孔表面領域上に配置されている多孔質界面層;
該第二細孔表面領域上に配置されたフィッシャー・トロプシュ触媒;及び 水素ガスと一酸化炭素ガスとの混合物を有する供給流を該触媒構造物に流し、該触媒構造物を、作業圧力において、少なくとも200℃まで加熱し、該供給流が、該触媒構造物内において5秒未満の滞留時間を有し、それにより、少なくとも25%の一酸化炭素転化率及びメタンへの選択率がせいぜい25%の生成物流を得る工程を有するフィッシャー・トロプシュ合成の方法も提供する。
CO及びH2の触媒転化に関する滞留時間及び反応温度の効果を、定流反応器(constat flow reactor)中で試験した。反応器には、モル比又は体積(理想気体挙動を仮定している)比H2/CO=3で、H2とCOとから成る供給ガスの混合物を供給した。この反応体供給物を、等温炉内にある一定温度に維持された反応チャンバー中に供給した。触媒チャンバーの内部は、長さ35.6mm(1.4インチ)、厚さ1.5mm(0.060インチ)及び幅8mm(0.315インチ)である。反応生成物は、反応チャンバーから出して、捕集し、組成を分析した。
実験を行って、様々な圧力での運転を実証した。装置は実施例1と同じであった。
金属フォーム上触媒として、酸性ガンマアルミナに担持されたCo又はRu単独使用を、実施例1の条件下で試験し、その性能が、例えばCo−Ruのようなバイメタル触媒の性能に比べて劣ることを見出した。
実験を行って、本発明の緩衝層のある種の利点を実証した。
エッチングされていないステンレス鋼フォーム(オハイオ州シンシナティにあるAstroMet)を、化学蒸着法によって、1000オングストロームのTiO2でコーティングした。チタンイソプロポキシド(マサチューセッツ州ニューバリーポートにあるStrem Chemical)を、0.1 〜 100トルの圧力、250 〜 800℃の温度で蒸着させた。フォームに対して優れた付着力を有するチタニアコーティングが、600℃の蒸着温度及び3トルの反応器圧で得られた。
本発明の好ましい態様を示し説明して来たが、本発明から逸脱せずに、多くの変更及び改良を成し得ることは、当業者には明らかである。而して、添付の請求の範囲は、本発明の真の精神及び範囲内にあるすべてのそのような変更及び改良に及ぶことを意図している。
Claims (14)
- 水素と一酸化炭素とを含む供給流を、少なくとも200℃の温度において、触媒を含む反応チャンバー中に流す工程;
担持された、コバルト、ルテニウム、鉄、レニウム、オスミウム及びこれらの組み合わせからなる群より選択されるフィッシャー・トロプシュ触媒金属を含む該触媒;
定常状態条件下で該供給流が2秒未満の接触時間を有するような充分な速度で、該反応チャンバーから該反応チャンバーと熱接触している冷却チャンバーへ熱を伝える工程;
生成物流を捕集する工程を含む一酸化炭素を水素化する方法であって、
前記反応チャンバーが板状であり、
前記冷却チャンバーが前記反応チャンバーに隣接しており、
前記反応チャンバーを通る供給流の流れ方向に直交しかつ前記冷却チャンバーへの熱の流れと平行な方向における前記触媒の厚みが1.5cm以下であって、
該触媒の断面積が前記反応チャンバーの断面積の少なくとも95%を占め、ここで前記反応チャンバーの断面積は前記反応チャンバーを通る供給流の流れ方向に直交しており、
該方法が:
25%未満のメタン選択率、
25%超の一酸化炭素転化率、及び
液体生成物の体積を20℃及び1気圧で測定する場合に、1分当たり液体生成物を少なくとも1ミリリットル含む生成速度、又は
ガス状生成物の体積を20℃及び1気圧で測定する場合に、生成物が分子1個当たり少なくとも2個の炭素原子を含むガス状炭化水素生成物を1分当たり少なくとも1リットル含む生成速度を有することを特徴とする前記方法。 - 炭化水素を生成する請求項1記載の方法。
- 該炭化水素が、室温及び1気圧で液体の燃料である請求項2記載の方法。
- 該触媒が、
第一細孔表面領域と、少なくとも0.1μmの第一細孔サイズとを有する金属、又はセラミックを含む多孔質担体;
第二細孔表面領域と該第一細孔サイズ未満の第二細孔サイズとを有し、窒化物、炭化物、硫化物、ハロゲン化物、金属酸化物、炭素及びこれらの組合せからなる群より選択される多孔質界面層であって、該第一細孔表面領域上に配置される該多孔質界面層;及び
該第二細孔表面領域上に配置される、コバルト、ルテニウム、鉄、レニウム、オスミウム及びそれらの組合せから成る群より選択されるフィッシャー・トロプシュ触媒を含む、請求項1に記載の方法。 - 該触媒が、前記多孔質担体とフィッシャー・トロプシュ触媒金属との間にAl2O3、TiO2、SiO2、及びZrO2又はそれらの組合せを含む緩衝層を備える、請求項4記載の方法。
- 該緩衝層がα−Al2O3を含む、請求項5記載の方法。
- 該触媒が、該緩衝層の上に金属酸化物の界面層を含む、請求項5記載の方法。
- 該触媒における該界面層が、50μm未満の深さを有する多孔質界面層である、請求項7記載の方法。
- 該触媒における該界面層が、20μm未満の深さを有する多孔質界面層である、請求項7記載の方法。
- 該触媒が1〜10mmの厚さを有する、請求項1記載の方法。
- 該触媒が反応チャンバー壁に接触している、請求項10記載の方法。
- 接触時間が0.1〜1秒である、請求項1記載の方法。
- 一酸化炭素の転化率が80%超であり、メタン選択率が20%未満である、請求項1記載の方法。
- 該フィッシャー・トロプシュ触媒金属が、コバルト、ルテニウム、鉄、レニウム、オスミウム及びそれらの組合せから成る群より選択され、かつコバルトを必須として含む、請求項1記載の方法。
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US09/492,254 US6558634B1 (en) | 1999-08-17 | 2000-01-27 | Catalyst structure and method of fischer-tropsch synthesis |
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ZA200200853B (en) | 2003-04-30 |
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US20020099103A1 (en) | 2002-07-25 |
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JP4805501B2 (ja) | 2011-11-02 |
US6491880B1 (en) | 2002-12-10 |
US6451864B1 (en) | 2002-09-17 |
EP1637219B1 (en) | 2017-11-29 |
NO20092105L (no) | 2002-04-09 |
US20060148910A1 (en) | 2006-07-06 |
EP2264128A2 (en) | 2010-12-22 |
US7585899B2 (en) | 2009-09-08 |
JP2003507176A (ja) | 2003-02-25 |
EP2264128B1 (en) | 2017-10-25 |
US7045486B2 (en) | 2006-05-16 |
US20040063799A1 (en) | 2004-04-01 |
EP1637219A2 (en) | 2006-03-22 |
US6660237B2 (en) | 2003-12-09 |
KR100666394B1 (ko) | 2007-01-09 |
NO20083130L (no) | 2002-04-09 |
NO331868B1 (no) | 2012-04-23 |
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