JP2012110894A - 触媒、その製造方法、及び触媒を用いる反応 - Google Patents
触媒、その製造方法、及び触媒を用いる反応 Download PDFInfo
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- JP2012110894A JP2012110894A JP2012005341A JP2012005341A JP2012110894A JP 2012110894 A JP2012110894 A JP 2012110894A JP 2012005341 A JP2012005341 A JP 2012005341A JP 2012005341 A JP2012005341 A JP 2012005341A JP 2012110894 A JP2012110894 A JP 2012110894A
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- B01J37/02—Impregnation, coating or precipitation
- B01J37/0215—Coating
- B01J37/0225—Coating of metal substrates
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/00781—Aspects relating to microreactors
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- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
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- B01J35/56—Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional monoliths
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T29/00—Metal working
- Y10T29/49—Method of mechanical manufacture
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Abstract
【解決手段】金属製チャネル壁面に直接、あるいは壁面をエッチングにより多孔質化した後、Al2O3、SiO2,ZrO2,TiO2及びこれらの組合せから選択される金属酸化物を含む緩衝層102を蒸着により形成させ、さらに溶液堆積法により金属酸化物を含有する界面層104を形成させ、この界面層の上に触媒層106を堆積させた、マイクロチャネル装置。
【選択図】図1
Description
多孔質担体は、金属又はセラミックのフォーム(foam)であることができる。金属フォームは、高度に熱伝導性であり、且つ機械加工し易い。スポンジ様の機械的性質により、機械的接触を介して反応室を簡便にシールすることができる。金属フォームと収容反応室(housing reaction chamber)との間の密接に適合させた熱膨張により、より高温において、多孔質担体のクラッキングが最小になり、また多孔質担体周囲のガスの偏流が最少になる。Pestryakovらは、n−ブタンを酸化するための中間ガンマ・アルミナ層を有する[1]及び有しない[2]金属フォーム担持遷移金属酸化物触媒を調製した。Kosak[3]は、表面をHCl溶液でプレエッチングする、様々な金属フォーム上に貴金属を分散させるためのいくつもの方法を試験し、無電解メッキが、フォーム担体に対して貴金属を最も良好に接着させることを報告した。Podyachevaら[4]も、メタンを酸化するための多孔質アルミナ中間層を有するフォーム金属担持LaCoO3ペロブスカイト触媒を合成した。金属フォーム担持触媒を用いることによるすべての潜在的な利点にもかかわらず、金属フォームは、耐蝕性が低く、その非多孔質及び滑らかなウエッブ表面に起因してセラミック材料に対する接着が不良であり、またこれらの材料は、熱膨張率が適合していないので、熱サイクル後に、界面層がスポーリングする傾向がある。
多孔質担体100は多孔質セラミック又は金属の形態であることができる。本発明での使用に適する他の多孔質担体としては、炭化物、窒化物、及び複合材料が挙げられる。層を堆積させる前、多孔質担体は、水銀圧入法によって測定した場合、少なくとも5%の多孔度を有し、また光学顕微鏡及び走査電子顕微鏡によって測定した場合、1μmから1000μmの平均細孔サイズ(孔径の合計/細孔数)を有する。多孔質担体は、好ましくは約30%から約99%の多孔度、更に好ましくは70%から98%の多孔度を有する。多孔質担体の好ましい形態は、フォーム、フェルト、ワッド(wad)及びそれらの組合わせである。フォームは、構造全体にわたって細孔を画定している連続壁を有する構造である。フェルトは、それらの間に隙間空間を有する繊維の構造である。ワッドは、スチールウールのような絡み合ったストランドの構造である。好ましさは劣るが、多孔質担体としては、上記の多孔度及び細孔サイズの特性を有するという条件付で、他の多孔質媒体、例えばペレット及びハニカムも挙げることかできる。金属フォームの連続気泡(open cells)は、好ましくは1インチ当たり細孔の個数が約20(ppi)から約3000ppi、更に好ましくは約40から約120ppiである。PPIは、1インチ当たりの細孔の最大個数と規定される(等方性材料では、測定方向は無関係であるが;異方性材料では、測定は細孔数が最大になる方向で行う)。本発明では、ppiは走査電子顕微鏡で測定する。多孔質担体は、低い圧力低下、従来のセラミックペレット担体を超える向上した熱伝導性、及び化学反応器におけるロード/アンロードのし易さを含む本発明におけるいくつもの利点を提供することを発見した。
実験を行って、本発明の緩衝層の確かな利点を証明した。
エッチングされていないステンレス鋼フォーム(オハイオ州ンシナティにあるAstromet)を、化学蒸着法によって、1000ÅのTiO2で被覆した。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トルから100トルの圧力で250℃から800℃の温度において、蒸着させた。600℃の堆積温度及び3トルの反応器圧において、該フォームに対して優れた接着を有するチタン被覆が得られた。
Claims (22)
- 多孔質担体、緩衝層、界面層、及び表面上に触媒活性層を含む触媒であって;該緩衝層が、該多孔質担体と該界面層との間に配置されていて、且つ該界面層が、該触媒活性層と該緩衝層との間に配置されている前記触媒。
- 多孔質担体、緩衝層、及び界面層を含む触媒であって;該緩衝層が、少なくとも2つの組成的に異なる副層を含み、且つ該緩衝層が、該多孔質担体と該界面層との間に配置されている前記触媒。
- 前記界面層上に触媒活性層を更に含む請求項2記載の触媒。
- 多孔質担体、緩衝層、及び界面層を含む触媒であって;該緩衝層が、該多孔質担体と該界面層との間に配置されていて;且つ該触媒が空気中で3回の熱サイクルに曝された場合に、該触媒が2%未満のフレーキングを示すように、該触媒が熱サイクル安定性を有する前記触媒。
- 前記多孔質担体が金属であって;且つ更に、前記触媒が空気中で580℃において2500分間加熱される場合に、該触媒が5%未満だけ重量が増加するように、該触媒が耐酸化性を有する請求項4記載の触媒。
- 以下の工程:すなわち、 多孔質担体を選択する工程;
該多孔質担体上に緩衝層を蒸着させる工程;
該緩衝層上に界面層を堆積させる工程を含む触媒を製造する方法。 - 少なくとも1つの反応体を反応室中へと通す工程;
その場合、該反応室は請求項1記載の触媒を含む;
該少なくとも1つの反応体を少なくとも1つの生成物へと転化させる工程;及び
該生成物を該反応室から外に出す工程を含む、少なくとも1つの反応体を少なくとも1つの生成物へと転化させる方法。 - 少なくとも1つの反応体を反応室中へと通す工程;
その場合、該反応室は請求項2記載の触媒を含む;
該少なくとも1つの反応体を少なくとも1つの生成物へと転化させる工程;及び
該生成物を該反応室から外に出す工程を含む、少なくとも1つの反応体を少なくとも1つの生成物へと転化させる方法。 - 少なくとも1つの反応体を反応室中へと通す工程;
その場合、該反応室は請求項3記載の触媒を含む;
該少なくとも1つの反応体を少なくとも1つの生成物へと転化させる工程;及び
該生成物を該反応室から外に出す工程を含む、少なくとも1つの反応体を少なくとも1つの生成物へと転化させる方法。 - 前記方法を:アセチル化、付加反応、アルキル化、脱アルキル化、水素化脱アルキル化、還元的アルキル化、アミノ化、芳香族化、アリル化、自熱式改質、カルボニル化、脱カルボニル化、還元的カルボニル化、カルボキシル化、還元的カルボキシル化、還元的カップリング、縮合、分解、水素化分解、環化、シクロオリゴマー化、脱ハロゲン化、二量体化、エポキシ化、エステル化、交換、フィッシャー・トロプシュ、ハロゲン化、水素化ハロゲン化、ホモログ化、水和、脱水、水素化、脱水素、ヒドロカルボキシル化、ヒドロホルミル化、水素化分解、ヒドロメタル化、ヒドロシリル化、加水分解、水素処理法、水素化脱硫/水素化脱窒素(HDS/HDN)、異性化、メタノール合成、メチル化、脱メチル化、メタセシス、ニトロ化、酸化、部分酸化、重合、還元、水蒸気改質及び二酸化炭素改質、スルホン化、テロメリゼーション、エステル交換反応、三量体化、水性ガス転化(WGS)、及び逆水性ガス転化(RWGS)から成る群より選択する請求項9記載の方法。
- 前記方法を:アセチル化、付加反応、アルキル化、脱アルキル化、水素化脱アルキル化、還元的アルキル化、アミノ化、芳香族化、アリル化、自熱式改質、カルボニル化、脱カルボニル化、還元的カルボニル化、カルボキシル化、還元的カルボキシル化、還元的カップリング、縮合、分解、水素化分解、環化、シクロオリゴマー化、脱ハロゲン化、二量体化、エポキシ化、エステル化、交換、フィッシャー・トロプシュ、ハロゲン化、水素化ハロゲン化、ホモログ化、水和、脱水、水素化、脱水素、ヒドロカルボキシル化、ヒドロホルミル化、水素化分解、ヒドロメタル化、ヒドロシリル化、加水分解、水素処理法、水素化脱硫/水素化脱窒素(HDS/HDN)、異性化、メタノール合成、メチル化、脱メチル化、メタセシス、ニトロ化、酸化、部分酸化、重合、還元、水蒸気改質及び二酸化炭素改質、スルホン化、テロメリゼーション、エステル交換反応、三量体化、水性ガス転化(WGS)、及び逆水性ガス転化(RWGS)から成る群より選択する請求項7記載の方法。
- 前記方法を:アセチル化、付加反応、アルキル化、脱アルキル化、水素化脱アルキル化、還元的アルキル化、アミノ化、芳香族化、アリル化、自熱式改質、カルボニル化、脱カルボニル化、還元的カルボニル化、カルボキシル化、還元的カルボキシル化、還元的カップリング、縮合、分解、水素化分解、環化、シクロオリゴマー化、脱ハロゲン化、二量体化、エポキシ化、エステル化、交換、フィッシャー・トロプシュ、ハロゲン化、水素化ハロゲン化、ホモログ化、水和、脱水、水素化、脱水素、ヒドロカルボキシル化、ヒドロホルミル化、水素化分解、ヒドロメタル化、ヒドロシリル化、加水分解、水素処理法、水素化脱硫/水素化脱窒素(HDS/HDN)、異性化、メタノール合成、メチル化、脱メチル化、メタセシス、ニトロ化、酸化、部分酸化、重合、還元、水蒸気改質及び二酸化炭素改質、スルホン化、テロメリゼーション、エステル交換反応、三量体化、水性ガス転化(WGS)、及び逆水性ガス転化(RWGS)から成る群より選択する請求項8記載の方法。
- 装置の内壁の少なくとも1つを、緩衝層で被覆したマイクロチャネル装置。
- 前記緩衝層上に配置された界面層を更に含む請求項13記載のマイクロチャネル装置。
- 前記緩衝層を蒸着させた請求項13記載のマイクロチャネル装置。
- 前記壁が、該反応室の少なくとも1つの壁を含み、且つ該界面層上に配置された触媒活性材料を更に含む請求項14記載のマイクロチャネル装置。
- 前記緩衝層が、チタニアである請求項6記載の方法。
- 前記触媒が空気中で3回の熱サイクルに曝された場合に、該触媒が2%未満のフレーキングを示すように、該触媒が熱サイクル安定性を有する請求項1記載の触媒。
- 前記触媒が空気中で580℃において2500分間加熱される場合に、該触媒が5%未満だけ重量が増加するように、該触媒が耐酸化性を有する請求項1記載の触媒。
- 前記反応室が壁を有し、且つ該壁の少なくとも1つに対して、その上に:
緩衝層;
界面層;及び
触媒活性層が配置されている請求項7記載の方法。 - 前記触媒が空気中で750℃において1500分間加熱される場合に、該触媒が0.5%未満だけ重量が増加するように、該触媒が耐酸化性を有する請求項1記載の触媒。
- 前記多孔質担体が金属であり、且つ前記触媒活性層が、該触媒を通過する反応体が該触媒を通る流路に沿って至る所で反応できるように、該触媒全体の表面上に分散される請求項1記載の触媒。
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Also Published As
Publication number | Publication date |
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RU2257955C2 (ru) | 2005-08-10 |
US7498001B2 (en) | 2009-03-03 |
CA2396144A1 (en) | 2001-08-02 |
EP2295140A1 (en) | 2011-03-16 |
EP1257362B1 (en) | 2013-05-08 |
CN1211162C (zh) | 2005-07-20 |
KR20020080387A (ko) | 2002-10-23 |
WO2001054812A1 (en) | 2001-08-02 |
AU3466601A (en) | 2001-08-07 |
AU2005200598A1 (en) | 2005-03-10 |
RU2002120794A (ru) | 2004-01-10 |
EP1257362A1 (en) | 2002-11-20 |
NO20023080D0 (no) | 2002-06-26 |
JP2003520675A (ja) | 2003-07-08 |
US20030007904A1 (en) | 2003-01-09 |
AU2005200598B2 (en) | 2007-12-20 |
JP5964594B2 (ja) | 2016-08-03 |
NO20023080L (no) | 2002-09-13 |
JP4982717B2 (ja) | 2012-07-25 |
US6440895B1 (en) | 2002-08-27 |
AU778052B2 (en) | 2004-11-11 |
US6762149B2 (en) | 2004-07-13 |
KR100670954B1 (ko) | 2007-01-17 |
HK1053996A1 (en) | 2003-11-14 |
CN1400923A (zh) | 2003-03-05 |
WO2001054812B1 (en) | 2001-11-29 |
AU778052C (en) | 2005-09-01 |
US20040188326A1 (en) | 2004-09-30 |
CA2396144C (en) | 2013-11-19 |
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