Autothermal reforming catalyst and process of producing fuel gas for fuel cell

a technology of autothermal reforming and fuel gas, which is applied in the direction of physical/chemical process catalysts, bulk chemical production, metal/metal-oxide/metal-hydroxide catalysts, etc., can solve the problems of catalyst development, low activity, and carbon precipitation, and achieve long working life, high activity, and not decreased effect of activity

Inactive Publication Date: 2003-03-27
NIPPON MITSUBISHI OIL CORP
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Benefits of technology

0057] The autothermal reforming catalyst of the present invention has an extremely high activity and long working life. However, in the case of continuing the use of the catalyst over a long period of time, if necessary, the catalyst is preferably subjected to a refresh treatment such as reduction under a reduction atmosphere, generally, a hydrogen atmosphere at a temperature of 400 to 1,000.degree. C., and preferably 500 to 700.degree. C.
0058] The autothermal reforming catalyst of the present invention is not decreased in activity even using ruthenium which has conventionally the tendency to be decreased in activity under an oxygen atmosphere at elevated temperatures, leading to a sufficient working life and can maintain the effect of suppressing carbon to precipitate at a lower steam / carbon ratio. Furthermore, since the catalyst comprises ruthenium which is cheaper among the noble metals, it is advantageous in the industrial use.

Problems solved by technology

The base metal-based catalysts are relatively prone to cause carbon precipitation.
However, these catalysts have a problem that they are expensive.
While ruthenium is relatively cheap, it is prone to de be decreased in activity due to volatilization in the case where oxygen coexists at elevated temperatures such as those at which an autothermal reforming reaction is conducted.
Therefor, there has been demanded a cheap catalyst which hardly cause the carbon to precipitate even under such a condition that the steam / carbon ratio is low in an autothermal reforming reaction so as to be able to produce hydrogen at high efficiency and is excelled in heat resistance under the coexistence of oxygen, but such a catalysts has not been developed yet.

Method used

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Examples

Experimental program
Comparison scheme
Effect test

example 1

[0060] (1) Preparation of Catalyst

[0061] .gamma.-alumina powder with a specific surface of 190 m.sup.2 / g was dipped into a water-soluble solution of cerium nitrate, and the water is evaporated therefrom. The powder was dried at a temperature of 120.degree. C. for 3 hours and then calcined in the air at a temperature of 800.degree. C. for 3 hours, thereby preparing a catalyst support.

[0062] The support was dipped into a water-soluble solution of ruthenium chloride, and then the water was evaporated therefrom. The support was dried at a temperature of 120.degree. C. for 3 hours. After the support was pressed, it was ground and sifted, thereby obtaining a granulated catalyst with a size of about 1 to 2 mm. The catalyst was reduced under a hydrogen circulation at a temperature of 500.degree. C. for 3 hours thereby obtaining Catalyst A. The chemical composition of Catalyst A is shown in Table 1.

[0063] (2) Autothermal Reforming Reaction

[0064] A reaction tube with an inner diameter of 9 mm...

example 2

[0069] (1) Preparation of Catalyst

[0070] .gamma.-alumina powder with a specific surface of 190 m.sup.2 / g was dipped into a water-soluble solution of cerium nitrate, and the water is evaporated therefrom. The powder was dried at a temperature of 120.degree. C. for 3 hours and then calcined in the air at a temperature of 800.degree. C. for 3 hours, thereby preparing a catalyst support. The support was dipped into a water-soluble solution of barium nitrate, and the water was evaporated therefrom. The support was dried at a temperature of 120.degree. C. for 3 hours and calcined in the air at a temperature of 800.degree. C. for 3 hours.

[0071] The support was dipped into a water-soluble solution of ruthenium chloride, and then the water was evaporated therefrom. The support was dried at a temperature of 120.degree. C. for 3 hours. After the support was pressed, it was ground and sifted, thereby obtaining a granulated catalyst with a size of about 1 to 2 mm. The catalyst was reduced under ...

example 3

[0076] (1) Preparation of Catalyst

[0077] .gamma.-alumina powder with a specific surface of 190 m.sup.2 / g was dipped into a water-soluble solution of cerium nitrate, and the water is evaporated therefrom. The powder was dried at a temperature of 120.degree. C. for 3 hours and then calcined in the air at a temperature of 800.degree. C. for 3 hours, thereby preparing a catalyst support. The support was dipped into a water-soluble solution of magnesium nitrate, and the water was evaporated therefrom. The support was dried at a temperature of 120.degree. C. for 3 hours and calcined in the air at a temperature of 800.degree. C. for 3 hours.

[0078] The support was dipped into a water-soluble solution of ruthenium chloride, and then the water was evaporated therefrom. The support was dried at a temperature of 120.degree. C. for 3 hours. After the support was pressed, it was ground and sifted, thereby obtaining a granulated catalyst with a size of about 1 to 2 mm. The catalyst was reduced und...

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Abstract

Autothermal reforming catalysts comprises ruthenium supported on a support containing 5 to 40 percent by mass of a cerium oxide or rare earth element oxide which is composed principally of a cerium oxide, 60 to 95 percent by mass of an aluminum oxide, and 0 to 10 percent by mass in terms of metal of one or more elements selected from the group consisting of an alkaline metal and an alkaline earth metal, the atomic ratio of cerium and rhodium (Ce/Rh) being 1 to 250.

Description

[0001] 1. Field of the Invention[0002] This invention relates to an autothermal reforming catalyst. This invention also relates to a process of producing a fuel gas for a fuel cell wherein hydrocarbons and / or oxygen-containing hydrocarbons are converted to a reformed gas which is composed principally of hydrogen by an autothermal reforming reaction using such a catalyst.[0003] 2. Description of the Prior Art[0004] A known process for producing hydrogen from hydrocarbons or oxygen-containing hydrocarbons is an autothermal reforming method which is the combination of an oxidation reaction and a steam reforming reaction. In this process, hydrocarbons or nitrogen-containing hydrocarbons, steam, and oxygen or air are introduced into a reactor, and a part of the hydrocarbons or oxygen-containing hydrocarbons is subjected to partial or complete combustion. While the reactor is then heated to a predetermined temperature with the heat generated by the combustion, the remaining hydrocarbons o...

Claims

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Application Information

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Patent Type & Authority Applications(United States)
IPC IPC(8): B01J23/58B01J23/63B01J35/10C01B3/32C01B3/40H01M8/06
CPCB01J23/63B01J35/10B01J35/1019C01B3/326C01B3/40C01B2203/0244C01B2203/066C01B2203/0844C01B2203/1064C01B2203/1082C01B2203/1205C01B2203/1217C01B2203/1235Y02P20/52
Inventor ANZAI, IWAOMATSUMOTO, TAKAYA
Owner NIPPON MITSUBISHI OIL CORP
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