JP2007525223A - 液体反応体から生成物を生成させる改良触媒方法 - Google Patents
液体反応体から生成物を生成させる改良触媒方法 Download PDFInfo
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Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
- B01J35/56—Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional monoliths
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- B—PERFORMING OPERATIONS; TRANSPORTING
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Abstract
Description
(a)入口端及び出口端が隣接流路によって接続されたセラミックハニカム中に反応体を含む液体を流入させ(ここで、隣接流路はセラミックハニカムの入口端から出口端に伸び;流路は、表面に触媒を有する複数の絡み合った薄い多孔質隔壁によって規定され;隔壁は、反応体を含む液体がモノリシック構造のセラミックハニカムの入口端から出口端まで流れる際に、反応体を含む液体が壁に実質的に浸透し且つ反応体が反応する気孔率を有する);そして
(b)セラミックハニカムの出口端から反応生成物を回収する
ことを含んでなる液体からの反応生成物の生成方法である。
(a)淀んでいると見なすことができる容器中の液体のフラクション(淀んだ液体フラクション)、
(b)淀んだ液体フラクションと動的液体フラクションとの間の交換(物質交換)の速度、及び
(c)不規則な速度の変動の振幅(ディスパージョン)。
触媒の量は、個々の反応に応じて任意の適当な量であることができる。一般に、セラミック粒子の少なくとも約10%〜本質的に全てが被覆されるか、又は触媒を含む。
例1〜23及び比較例1〜8においては、管壁とサンプルとの間の液体のバイパスを防止し且つ2つのサンプル間の空間が2mm未満となるように、垂直に取り付けた管中に直径約4cmのセル400個/inch2を有するハニカムを積み重ねた。水及び空気を、カラムの最上部でサンプルの断面全体に均一に分布させ、カラムを通して下方に向かって所定の流量で強制的に流した。検出可能なトレーサーを、サンプルを含むカラムの真上で液体供給材料中に注入した。トレーサーは、カラム内部の液体の滞留時間に比較して短い期間で注入した。管中の最後のサンプルの真下において、容器から出る液体の経時的濃度を、検出可能なトレーサーがカラム流出液中において検出されなくなるまで記録した。出口濃度対時間のデータを、曲線の下の面積及び曲線の最初の瞬間を用いて正規化して、いわゆるE(シータ)曲線を得た。
セル200個/inch2の針状ムライトハニカム(気孔率60%)、直径4.3cm×長さ5cmを、65%スクロース水溶液中に室温で5分間浸漬した。含浸後、過剰の溶液を、流路に空気を吹き込むことによって流路から除去した。サンプルを連続回転下で室温において24時間乾燥させた後、393ケルビン(K)で3時間乾燥させた。サンプルを、水平炉中に配置された管型石英反応器中で炭化させた。サンプルは管型石英反応器中でN2流中において823Kまで10K/分で加熱した。サンプルを500mL/分のN2流下で823Kに2時間保持して、炭化担体を調製した。炭化後、担体は、重量増加によって計算すると、炭素が15重量%であった。
フルフリルアルコール(90mL)及びピロール(27mL)を293Kにおいて攪拌した。酸触媒(7mL、65% HNO3)を45分間にわたって徐々に添加した。この発熱反応の間、氷浴を用いて温度を293Kの一定に保った。重合を293Kにおいて1時間続けた。
Nijhuisら,Chemical Engineering Science,56(3),823−829(2001)によって記載された方法によって、炭素ナノファイバーをベースとするコーティングを製造した。Puralox SBA 200 γ−アルミナ(Condea)300g及びコロイドアルミナ(水中20%,Alfa Aesar)170gを水400mL中で混合した。pHを硝酸で4.5に調整し、スラリーを24時間ボールミル磨砕した。pHを硝酸で再び4.5に調整した。セル200個/inch2の針状ムライトハニカム(気孔率60%)、直径4.3cm×長さ5cmを、スラリー中に5分間浸漬し、水平にしてゆっくりと回転させながら乾燥させた。サンプルを723Kにおいて4時間焼成した。ニッケルを、353Kにおいて1M尿素水溶液から担体上に沈着(付着)させた。973Kにおいて1時間還元後、炭素ナノファイバーを石英反応器中で、Kovalenkoらの方法(Journal of Molecular Catalysis A: Chemical,182−183,73−80(2002))に従って生長させた。Ni含浸サンプルをN2流中において973Kまでで加熱した(10K/分)。ニッケルをN2中20%H2中で1時間還元させた。773〜873Kに冷却後、炭素繊維を、プロペン又はメタン中及びN2中H2中で生長させた(総流量200mL/分)。担体は、重量増加によって計算すると、炭素を6重量%含んでいた。
セル200個/inch2の針状ムライトハニカム(気孔率60%)、直径4.3cm×長さ5cmを、40%水性コロイドシリカ懸濁液(Ludox AS−40,Aldrich)中に5分間浸漬した。過剰の液体を、流路からゆるやかに吹き飛ばし、サンプルを空気中で一晩乾燥させてから、723Kにおいて4時間焼成した。次いで、サンプルをN−[3−(トリメトキシシリル)プロピル]ポリエチレンイミンヒドロクロリド(Aldrich)の2−プロパノール中10%(v/v)溶液中に45時間浸漬して置いた。この浸漬後、サンプルを2−プロパノールで2回、水で2回洗浄した。
Claims (20)
- (a)セラミックハニカムの入口端から出口端に伸びる隣接流路によって接続された、入口端及び出口端を有するセラミックハニカム中に、反応体を含む液体を流入させ(ここで前記流路は、表面に触媒を有する複数の絡み合った薄い多孔質隔壁によって規定され;前記隔壁は、反応体を含む液体がモノリシック構造のセラミックハニカムの入口端から出口端まで流れる際に、反応体を含む液体が壁に実質的に浸透し且つ反応体が反応する気孔率を有する);そして
(b)セラミックハニカムの出口端から反応生成物を回収する
ことを含んでなる液体からの反応生成物の生成方法。 - 前記モノリスセラミックハニカムが、少なくとも約50%の気孔率及び少なくとも約5μmの平均気孔寸法を有する請求項1に記載の方法。
- 反応体を含む液体が、液体中にパルス化されるトレイサーのTaylor流下で得られる滞留時間分布を用いて測定された場合に、静止液体フラクションの少なくとも10%である量で浸透する請求項1に記載の方法。
- 前記量が、静止液体フラクションの少なくとも約15%である請求項3に記載の方法。
- 前記方法が、E−曲線を用いて計算した場合に少なくとも約0.4の物質交換を有する請求項4に記載の方法。
- 前記物質交換が少なくとも約0.7である請求項5に記載の方法。
- 前記静止液体フラクションが少なくとも約1.25である請求項6に記載の方法。
- 前記触媒が酵素を含む請求項1に記載の方法。
- 前記触媒が貴金属、卑金属又はそれらの組合せを含む請求項1に記載の方法。
- 前記反応体の少なくとも1種を、気体として導入する請求項1に記載の方法。
- 前記反応体の少なくとも1種が液体と同時に流れる気泡中の気体である請求項1に記載の方法。
- 前記液体が溶解された反応体を有する溶媒を含む請求項1に記載の方法。
- 前記溶媒が水である請求項12に記載の方法。
- モノリシック構造の前記セラミックハニカムが針状セラミックである請求項1に記載の方法。
- 前記針状セラミックが少なくとも約3μmの平均気孔寸法及び少なくとも約2のアスペクト比を有する請求項1に記載の方法。
- 前記針状セラミックが少なくとも約5μmの平均気孔寸法を有する請求項15に記載の方法。
- 前記針状セラミックが針状ムライトである請求項15に記載の方法。
- 前記触媒が炭素を含む請求項1に記載の方法。
- 前記炭素が炭素繊維である請求項18に記載の方法。
- 前記触媒が更に酵素を含む請求項19に記載の方法。
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JP2013063422A (ja) * | 2011-09-15 | 2013-04-11 | Ngk Insulators Ltd | ハニカム構造体 |
US9346003B2 (en) | 2011-09-15 | 2016-05-24 | Ngk Insulators, Ltd. | Honeycomb structure |
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MX2009004622A (es) | 2006-11-01 | 2009-05-15 | Dow Global Technologies Inc | Cuerpos porosos con forma de alfa-alumina y metodos para la preparacion de los mismos. |
DE102007040782A1 (de) * | 2007-08-28 | 2009-03-05 | GJ Research & Engineering Ltd., Wakefield | Verfahren und Vorrichtung zum Herstellen eines Biodiesel-Kraftstoffes |
US8425830B2 (en) * | 2008-02-29 | 2013-04-23 | Corning Incorporated | Permeable material, articles made therefrom and method of manufacture |
WO2010126680A2 (en) | 2009-04-29 | 2010-11-04 | Dow Technology Investments Llc | Porous body precursors, shaped porous bodies, processes for making them, and end-use products based upon the same |
JP6712732B2 (ja) * | 2018-09-11 | 2020-06-24 | 株式会社キャタラー | ファインバブルを用いた反応装置及び反応方法 |
CN109735528A (zh) * | 2019-02-27 | 2019-05-10 | 天津大学 | 用于染料降解的整体型生物反应器的制备方法 |
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