JPS60232245A - Preparation of monolithic type catalyst for converting carbon monoxide - Google Patents
Preparation of monolithic type catalyst for converting carbon monoxideInfo
- Publication number
- JPS60232245A JPS60232245A JP59086150A JP8615084A JPS60232245A JP S60232245 A JPS60232245 A JP S60232245A JP 59086150 A JP59086150 A JP 59086150A JP 8615084 A JP8615084 A JP 8615084A JP S60232245 A JPS60232245 A JP S60232245A
- Authority
- JP
- Japan
- Prior art keywords
- catalyst
- carbon monoxide
- nitrate hydrate
- present
- base material
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
Classifications
-
- 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
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts
Abstract
Description
【発明の詳細な説明】
（本発明の技術分野）
本発明は一酸化炭素転化反応に用いるモノリス型触媒の
製造法に関する。DETAILED DESCRIPTION OF THE INVENTION (Technical Field of the Invention) The present invention relates to a method for producing a monolithic catalyst used in a carbon monoxide conversion reaction.
（従来技術の概要）
今日の市民生活にとって都市ガスは欠くべからざるもの
となっている。従来から都市ガスの原料として用いられ
てきた石炭ならびに石油類が大都市およびその周辺部に
おいては液化石油ガスや液化天然ガスに置き換えられつ
つあるが、中小の都市においては石油改質ガスがいまだ
に主流をなしている。この改質ガスは毒性を有する一酸
化炭素を含有しているため、該−酸化炭素の含有量を低
減することが各方面から強く望まれておシ、現行のプロ
セスにおいては下記の接触反応により一酸化炭素の低減
がなされてい前記フ“ロセスにおいては、一般にベレッ
ト状に成型した酸化鉄−酸化クロム系触媒を光填し次固
定床式反応器により一酸化炭素転化反応が行われている
が、改質ガスが転化反応器を通過する際の圧力損失が大
きく、さらに、触媒ペレットの粉化によって経時的に圧
力損失が増大するという問題が生ずる。転化反応器での
圧力損失はガス移送に要する動力費増大の原因となるた
め、改質ガス製造業界においては上記の問題点を解決す
る触媒の開発が望まれている。(Summary of conventional technology) City gas has become indispensable for today's citizen life. Coal and petroleum, which have traditionally been used as raw materials for city gas, are being replaced by liquefied petroleum gas and liquefied natural gas in large cities and their surrounding areas, but reformed petroleum gas is still the mainstream in small and medium-sized cities. is doing. Since this reformed gas contains carbon monoxide, which is toxic, there is a strong desire from various quarters to reduce the content of carbon monoxide, and in the current process, the following catalytic reaction In the process where carbon monoxide is reduced, generally an iron oxide-chromium oxide catalyst shaped into a pellet is filled with light and then the carbon monoxide conversion reaction is carried out in a fixed bed reactor. , there is a problem that the pressure loss is large when the reformed gas passes through the conversion reactor, and the pressure loss increases over time due to the pulverization of the catalyst pellets.The pressure loss in the conversion reactor is caused by the gas transfer. Since this causes an increase in the required power cost, the reformed gas production industry is seeking the development of a catalyst that solves the above problems.
（本発明の目的）
本発明は従来の触媒の有する欠点全解消しうる一酸化炭
素転化用触媒の製造法全提供せんとするものである。(Objective of the present invention) The present invention aims to provide a complete method for producing a carbon monoxide conversion catalyst that can overcome all the drawbacks of conventional catalysts.
（本発明の構成）
本発明は少なくとも硝酸鉄水和物と硝酸クロム水和物と
を含む混合物の溶融ｇを耐熱性基材に含浸させたのち乾
燥および焼成を行うことを特徴とする一酸化戻累転化用
モノリス型触媒の製造法￥ｒ要旨とするものである。(Structure of the present invention) The present invention is characterized in that a heat-resistant base material is impregnated with a molten g of a mixture containing at least iron nitrate hydrate and chromium nitrate hydrate, and then dried and fired. This is a method for producing a monolithic catalyst for back-cycle conversion.
本発明でいう一酸化炭素転化用モノリス型触媒とは、単
一の形態を有する一酸化炭素転化用触媒であって、例え
ば１個１７′ｃはそｔ″Ｌ、以上のセットとなってガス
流動チャンネルを与える板状、中９円筒状または第１図
、第２図および第５図に示すような形態を有する一酸化
炭素転化用触媒がこれに相当する。なお第１〜３図にお
いてａは基材、ｂはガス流動チャンネルを示す。The monolithic catalyst for converting carbon monoxide as used in the present invention refers to a catalyst for converting carbon monoxide having a single form. This corresponds to a carbon monoxide conversion catalyst having a plate shape, a cylindrical shape, or a shape as shown in FIGS. 1, 2, and 5 that provide flow channels. indicates the base material, and b indicates the gas flow channel.
触媒製造用基材としてはガラス、アスベスト、ムライト
、ケイ酸カルシウム等の繊維の織布または不織布、コー
ジェライト、ムライト、アルミナ、チタニア等の多孔質
セラミックス類が用いられる。As the substrate for producing the catalyst, woven or nonwoven fabrics of fibers such as glass, asbestos, mullite, and calcium silicate, and porous ceramics such as cordierite, mullite, alumina, and titania are used.
本発明の一酸化炭素転化用モノリス型触媒は酸化鉄と酸
化クロムと全活性成分とするものであり、基材と活性成
分の量的関係は、基材１００重量部に対して酸化鉄と酸
化クロムの総重量が２重量部以上、好ましくは５〜３０
重量部であシ、かつ酸化鉄に対する酸化クロムの重量比
が０．０３〜αＢ、好ましくはα０５〜０．２である。The monolithic catalyst for carbon monoxide conversion of the present invention has iron oxide and chromium oxide as the total active components, and the quantitative relationship between the base material and the active components is such that iron oxide and chromium oxide are used for 100 parts by weight of the base material. The total weight of chromium is 2 parts by weight or more, preferably 5 to 30 parts by weight.
The weight ratio of chromium oxide to iron oxide is 0.03 to αB, preferably α05 to 0.2.
触媒の一般的な製造法は次のとおりである。A general method for producing a catalyst is as follows.
Ｆｅ（ＮＯ３）３ ・９Ｈ２０と０ｒ（ＮＯ３）３ ”
９Ｈ２０’ｆｆ含む混合物（Ｆｅ （Ｎ０３）３ ”
９ Ｎ２０に対する０ｒ（ＮＯ３）３’９Ｈ２０の重量
比が［１０３〜α８３、好ましくは０．０５〜Ｑ、２１
）全７０〜１００℃で加熱溶融し、この溶融液に基材上
浸漬することにより該溶融液を基材に含浸させ、次いで
５０〜１５０℃で乾燥させる。溶融液の含浸量は基材の
性状に依存するので、必要に応じて浸漬、乾燥を繰り返
したのち、２５０〜５００℃、好ましくは３００〜３５
０℃で焼成を行う。Fe(NO3)3 ・9H20 and 0r(NO3)3 ”
9H20'ff containing mixture (Fe (N03)3''
9 The weight ratio of Or(NO3)3'9H20 to N20 is [103 to α83, preferably 0.05 to Q, 21
) The base material is heated and melted at a total temperature of 70 to 100°C, and the base material is impregnated with the melt by dipping the base material into the melt, and then dried at a temperature of 50 to 150°C. The amount of impregnation with the melt depends on the properties of the base material, so after repeating dipping and drying as necessary, the temperature is 250 to 500°C, preferably 300 to 35°C.
Calcination is performed at 0°C.
次に本発明を実施例によってさらに説明する。Next, the present invention will be further explained by examples.
実施例
ペレット状触媒および本発明の方法で製造した触媒につ
き、活性ならびに触媒層における圧力損失特性の比較を
行った。The activity and pressure loss characteristics in the catalyst layer were compared between the pelletized catalyst of the example and the catalyst produced by the method of the present invention.
ベレット状触媒については、酸化鉄−酸化クロム系の市
販品（９，５■φＸ ＆ Ｏｍ ）全中空円筒型触媒層
（充填断面積１６．４ｍ２、長さ１６ｍ）が２段直列に
装填された反応器に充填し、表−１に示す条件下で一酸
化炭素転化反応金行った。Regarding the pellet-shaped catalyst, two commercially available iron oxide-chromium oxide type catalyst beds (9,5 φ The reactor was filled and a carbon monoxide conversion reaction was carried out under the conditions shown in Table 1.
−万、本発明の方法による触媒の製造は次のように行っ
た。断面１ ｍ２あたり３５，０００個のガス流動チャ
ンネルを有する断面７５ｗＸ７５ｍｍ、長さ５００腿の
コージェライト製基材會、Ｆｅ （ＮＯ３）３ ・９
Ｈ２０と０ｒ（ＮＯ３）３ ・９Ｈ２０との混合物（Ｆ
ｅ（ＮＯ３）３ ・９Ｈ２０に対するＯｒ （Ｎ０３）
３ ” ９Ｈ２０の重量比はα１）ｔ−８０℃に加熱し
て得た溶融液に１５分間浸漬したのち、１１０℃で１２
時間乾燥を行った。上記の浸漬、乾燥をさらに２回縁９
返したのち、５００℃で６時間の焼成を行い、酸化鉄お
よび酸化クロムの含有率が１０，５ｗｔ％のモノリス型
触媒を得た。この触媒６個を直列に装填した反応益金用
いて表−１に示す条件下で一酸化炭素転化反応金行った
。-Manufacturing of the catalyst by the method of the present invention was carried out as follows. Cordierite substrate with a cross section of 75w x 75 mm and a length of 500 mm with 35,000 gas flow channels per 1 m2 of cross section, Fe (NO3)3 9
A mixture of H20 and 0r(NO3)3 ・9H20 (F
e(NO3)3 ・Or (N03) for 9H20
The weight ratio of 3'' 9H20 is α1) After immersing it in the melt obtained by heating to t-80℃ for 15 minutes, it was heated to 110℃ for 12
Drying was performed for hours. Repeat the above soaking and drying two more times.
After returning the mixture, it was calcined at 500° C. for 6 hours to obtain a monolithic catalyst containing 10.5 wt % of iron oxide and chromium oxide. A carbon monoxide conversion reaction was carried out under the conditions shown in Table 1 using a reaction mixture containing six of these catalysts loaded in series.
表−１反応条件
なお、原料ガスの組成は、ペレット状触媒會用いた場合
、本発明の方法で製造した触媒を用いた場合のいずれも
、表−２のとおシである。Table 1 Reaction Conditions The composition of the raw material gas is as shown in Table 2, both when a pellet catalyst is used and when the catalyst produced by the method of the present invention is used.
表−２原料ガス組成
ベレット状触媒を用いた場合ならびに本発明の方法で製
造した触媒を用いた場合について、触媒装填時および触
媒装填後１０，０００時間を経過した時点での反応器出
口ガス中の一酸化炭素濃度、−酸化炭素転化率および触
媒層での圧力損失を表−６に示す。Table 2 Raw material gas composition In the case of using a pellet-shaped catalyst and the case of using a catalyst manufactured by the method of the present invention, in the reactor outlet gas at the time of catalyst loading and at the time of 10,000 hours after catalyst loading. Table 6 shows the carbon monoxide concentration, -carbon oxide conversion rate, and pressure loss in the catalyst layer.
表−３−酸化炭素転化反応の実施結果
ベレット状触媒と同様に、本発明の方法で製造した触媒
についても長期間にわたって初期活性が維持され、さら
にベレット状触媒を上回る一酸イし炭素転化率が達成さ
ｎていることは表−３に示した結果から明らかである。Table 3 - Results of carbon oxide conversion reaction Similar to the pellet-shaped catalyst, the catalyst produced by the method of the present invention maintains its initial activity for a long period of time, and furthermore, the monooxygen carbon conversion rate exceeds that of the pellet-shaped catalyst. It is clear from the results shown in Table 3 that this has been achieved.
−万、ペレット状触媒全用いた場合には触媒装填後１０
，０００時間を経過した時点で触媒層での圧力損失が触
媒装填時の３倍以上に増大しているのに対し、本発明の
方法で製造し次触媒を用いた場合には触媒装填時の圧力
損失がベレット状触媒を用いた場合よりも小さく、触媒
装填後１０．０００時間全経過した時点においても圧力
損失の増大が認められない。-10,000, 10,000 after loading the catalyst if all the pellet catalyst is used
,000 hours have elapsed, the pressure loss in the catalyst layer has increased to more than three times that of the time when the catalyst was loaded, whereas when the next catalyst manufactured by the method of the present invention was used, the pressure loss at the time of catalyst loading increased. The pressure loss is smaller than when a pellet-shaped catalyst is used, and no increase in pressure loss is observed even after 10,000 hours have passed after loading the catalyst.
（本発明の効果）
以上詳述したとおり、本発明の方法で製造した触媒は一
酸化炭素転化反応において従来のベレット状触媒と比較
して遜色のない活性含水し、従来のベレット状触媒を使
用し友場合に触媒層での圧力損失が経時的に増大すると
いう問題音解決するものであり、ガス移送に要する動力
費の低減に有効である。(Effects of the present invention) As detailed above, the catalyst produced by the method of the present invention has an active water content comparable to that of the conventional pellet-shaped catalyst in the carbon monoxide conversion reaction, and the catalyst produced by the method of the present invention has a water content comparable to that of the conventional pellet-shaped catalyst. This solves the problem of pressure loss in the catalyst layer increasing over time in the case of a catalytic converter, and is effective in reducing power costs required for gas transfer.
（本発明の適用分野）
なお、本発明の方法で製造した触媒は燃料電池用水嵩製
造用、アンモニア合成用水軍製造用等の水性ガス転化反
応においても有効な触媒であり、都市ガス製造用に限定
されるものではない。(Field of application of the present invention) The catalyst produced by the method of the present invention is also an effective catalyst in water gas conversion reactions such as for producing water bulk for fuel cells and for producing water for ammonia synthesis, and is suitable for producing city gas. It is not limited.
第１図、第２図および第３図は基材の形態全例示する図
である。
復代理人 内 １） 明
復代理人 萩 原 亮 −
第１図 第２図FIG. 1, FIG. 2, and FIG. 3 are diagrams showing all examples of the forms of the base material. Sub-Agents 1) Meifu Agent Ryo Hagiwara - Figure 1 Figure 2
Claims (1)
合物の溶融液を耐熱性基材に含浸させたのち乾燥および
焼成を行うことを特徴とする一酸化炭素転化用モノリス
型触媒の製造法。A method for producing a monolithic catalyst for carbon monoxide conversion, comprising impregnating a heat-resistant base material with a melt of a mixture containing at least iron nitrate hydrate and chromium nitrate hydrate, followed by drying and calcination. .
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59086150A JPS60232245A (en) | 1984-05-01 | 1984-05-01 | Preparation of monolithic type catalyst for converting carbon monoxide |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59086150A JPS60232245A (en) | 1984-05-01 | 1984-05-01 | Preparation of monolithic type catalyst for converting carbon monoxide |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPS60232245A true JPS60232245A (en) | 1985-11-18 |
Family
ID=13878704
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP59086150A Pending JPS60232245A (en) | 1984-05-01 | 1984-05-01 | Preparation of monolithic type catalyst for converting carbon monoxide |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS60232245A (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2008087115A2 (en) * | 2007-01-16 | 2008-07-24 | Basf Se | Method for producing a multi-element oxide material containing the element iron in the oxidised form |
-
1984
- 1984-05-01 JP JP59086150A patent/JPS60232245A/en active Pending
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2008087115A2 (en) * | 2007-01-16 | 2008-07-24 | Basf Se | Method for producing a multi-element oxide material containing the element iron in the oxidised form |
| WO2008087115A3 (en) * | 2007-01-16 | 2009-04-09 | Basf Se | Method for producing a multi-element oxide material containing the element iron in the oxidised form |
| JP2010515564A (en) * | 2007-01-16 | 2010-05-13 | ビーエーエスエフ ソシエタス・ヨーロピア | Method for producing multi-element oxide material containing iron element in oxidized form |
| US8128904B2 (en) | 2007-01-16 | 2012-03-06 | Basf Aktiengesellschaft | Process for preparing a multielement oxide composition comprising the element iron in oxidic form |
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