Catalyst – solid sorbent – or support therefor: product or process – Catalyst or precursor therefor – Metal – metal oxide or metal hydroxide
Reexamination Certificate
1997-11-26
2001-06-05
Yildirim, Bakir L. (Department: 1764)
Catalyst, solid sorbent, or support therefor: product or process
Catalyst or precursor therefor
Metal, metal oxide or metal hydroxide
C502S066000, C502S071000, C502S259000, C502S328000, C502S330000, C502S514000
Reexamination Certificate
active
06242380
ABSTRACT:
FIELD OF THE INVENTION
The present invention relates to a process for preparing supported nickel catalyst for reforming hydrocarbons. In particular, the present invention relates to a process for preparation of nickel catalyst supported on silicon and/or alumina-containing support for reforming hydrocarbons by using carbon dioxide and if desired, steam and/or oxygen as an oxidant.
BACKGROUND OF THE INVENTION
Supported nickel catalysts are widely used in reduction reaction such as reforming reaction, hydrogenation and methanation for their high activity of nickel metal, and thus are industrially very important. In particular, supported nickel catalysts are used for steam reforming of natural gas, oil and naphtha, and thus for producing synthesis gas which is major starting material of C1-chemistry in chemical industry. These catalysts are also used in the production of synthesis gas which is raw material of methanol, ammonia and oxygen-containing compounds.
Examples of the processes for preparing supported nickel catalysts generally include co-precipitation, impregnation, ion exchange, precipitation-deposition, sol-gel, and aerogel methods. The propertiess of the catalysts vary depending on the method of preparation and treatment of the nickel catalysts.
German Patent Laid-Open Publication No.2,255,909 disclosed that Ni
6
Al
2
(OH)
16
CO
3
4H
2
O, a precursor of catalyst, was prepared by co-precipitation method, and then Ni-Al type catalyst was prepared by calcining the precursor and the catalyst was used for steam reforming reaction of naphtha. Another German Patent Laid-Open Publication No.2,024,282 disclosed that supported nickel catalyst which was steam reforming catalyst of methane was prepared by a co-precipitation method comprising adding Na
2
CO
3
to an aqueous solution containing 15.3% of Ni(NO
3
)
2
6H
2
O and 7.6% of Al (NO
3
)
2
9H
2
O.
Japanese Patent Laid-Open Publication No.57-156,303 suggested a method of loading a nickel metal component by an impregnating method on natural zeolite. In the specification, natural zeolite was added to a 1 molar of aqueous solution of Ni(NO
3
)
2
, impregnated at 100° C. for one hour and then calcined at 400° C. for one hour. The prepared catalyst has a higher activity than that of a general nickel catalyst supported on alumina when used in the steam reforming reaction of natural gas.
Generally, supported nickel catalysts are mostly prepared by wet methods. However, these wet methods have problems that they require a drying step and acidic or basic waste water may be formed depending on preparing method. Therefore, these methods are difficult to apply the process industrially.
The present inventors have carried out extensive studies in order to solve the problems of the known wet methods and to find a process for preparing a supported nickel catalyst for reforming hydrocarbons with high activity without having a drying step and waste water problem. As a result, the present inventors have now found that by mixing a nickel salt and, if necessary, an alkali metal salt and/or alkaline earth metal salt with a silicon and/or aluminum-containing a support such as zeolite, silica and alumina, decomposing metal salts while melting all the salts and calcining the decomposed metals at 300° C. to 1200° C., supported nickel catalysts can be produced. The present invention has been attained on the basis of this finding.
SUMMARY OF THE INVENTION
It is an object of the present invention to provide a process for preparing supported nickel catalyst having high activity for reforming methane which not only can be used in place of expensive noble metal-supported catalyst but also can eliminate a drying step and waste water problems.
It is another object of the present invention to provide a process for preparing supported nickel or alkali metal and/or alkaline earth metal-promoted nickel catalysts which have high activity in the reforming reaction of hydrocarbons using carbon, dioxide,and, if desired, steam and/or oxygen as an oxidant.
In an aspect of the present invention, there is provided a process for preparing supported a nickel catalyst, which comprises-mixing a nickel salt having a low melting point of 100° C. or less and, if necessary, alkali metal salt and/or alkaline earth metal salt with silicon and/or aluminum-containing support such as zeolite, silica and alumina having surface area of 100 m
2
/g or more, decomposing metal salts while melting all the salts by heating them to a temperature above the melting points of the salts and then calcining the decomposed metal salts at 300° C. to 1200° C.
Other objects and advantages will be apparent to those who have ordinary skill in the art from the following description.
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patent: 4026823 (1977-05-01), Van Hook et al.
patent: 4042615 (1977-08-01), Vannice et al.
patent: 4209424 (1980-06-01), Le Goff et al.
patent: 4284531 (1981-08-01), Simpson et al.
patent: 4772750 (1988-09-01), Habermann
patent: 5130114 (1992-07-01), Igarashi
patent: 57-156303 (1982-09-01), None
J. Chem. Soc. Faraday Trans., 1994, 90(1), 193-202 Influence of Prep. Method on the Acidity of MoO3WO3)/ZrO2Catalysts. Afanasiev, Genatet, Breysse, Coudurier, Vedrine.
Chang Jong-San
Lee Kyu-Wan
Park Sang-Eon
Korea Research Institute of Chemical Technology
Ladas & Parry
Yildirim Bakir L.
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