Catalyst for conversion of methane to ethylene, preparation ther

Chemistry of hydrocarbon compounds – Unsaturated compound synthesis – By addition of entire unsaturated molecules – e.g.,...

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585500, 585943, 585652, 585651, 585513, 502 66, 502 74, 502161, 502162, 502208, 502164, 502210, 502166, 502213, 502171, C07C 224, B01J 2718, B01J 27185, B01J 2375

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056251076

DESCRIPTION:

BRIEF SUMMARY
FIELD OF THE INVENTION

The present invention relates to supported catalyst for converting methane into ethylene, preparation thereof, and process for manufacturing ethylene using said catalyst. More particularly, the present invention relates to a new catalyst which is expressed in the following general formula (1) for conversion reaction, preparation thereof, and process for preparation of ethylene by converting directly methane or methane-containing gas in the presence of the above catalyst.
M is a metal cluster or metal complex compound selected from the group of VIII, VII and VI elements;
S is an inorganic carrier such as SiO.sub.2 ;
P is a promoter of phosphorus compound;
D is a cobalt compound such as CoCl.sub.2 ;
"a" is weight percentage of metal cluster or metal complex compound in catalyst, having a value of 0.01 to 10; "c" is weight percentage of promoter in catalyst, ranging from 1.0 to 35.0.


BACKGROUND OF THE INVENTION

In general, ethylene has been widely used as one of the basic reaction chemicals in the field of petrochemical industry and fine chemical industry. It is well known that synthesis of ethylene from methane by dehydrogenation is conducted at relatively high temperature of about 1500.degree. to 1550.degree. C. through thermal or electric cracking reaction process.
However, this method causes some problems such as loss of an enormous amount of thermal energy and necessity of using high temperature equipment, and particularly severe corrosion of the reactor owing to high temperature.
As prior art describing synthesis of hydrocarbons by oxidative coupling and dehydrogenation in order to prepare lower hydrocarbons such as ethylene having a double bond by direct conversion of 5118654, Canadian Patent No. 2016675 and Japanese Patent Nos. 04352730, 04368342.
Above-referenced processes have more or less settled some disadvantages since the reaction is conducted at relatively lower temperature of about 700.degree. to 800.degree. C. However, since the reaction is conducted with oxygen, helium, nitrogen and N.sub.2 O as oxidation or dilution gas, variety of reactants and a large amount of by-proudcts such as CO.sub.2 are ensuing. Moreover, there are much difficulties in separating or purifying the reactants, let alone the inability to conduct a continuous process and the causation of a severe environmental pollution problem.
In the meantime, natural gas contains impurities such as carbon dioxide, H.sub.2 S and moisture other than methane as the major ingredient. These impurities may affect catalytic activity, if they are not purified and the reaction cannot proceed properly.


SUMMARY OF THE INVENTION

In order to be free of said disadvantages associated with the above-referenced processes, it is therefore an object of the present invention to provide a method for preparation of high-yield ethylene with an available continuous process at relatively lower temperature in the presence of the catalyst, without generation of by-products such as carbon dioxide. Another object of the present invention is to provide a direct and continuous conversion method of methane containing some impurities, such as natural gas, to ethylene. A further object of the present invention is to provide a new catalyst used in said process and preparation thereof.
To fulfill said object, an intensive study has been made by the inventor and it is found that the conversion catalyst may be made available through the following process:
By the operation of converting methane or methane-containing gas directly in the presence of the catalyst expressed as said general formula (1) at a temperature of 350.degree. to 1050.degree. C., ethylene with high yield may be obtained without by-products such as carbon dioxide. Also, by the operation of adding solvent to the components of said general formula (1), suspended, agitated in reflux at a temperature of about 20.degree. to 200.degree. C., evaporated residues by distillation under reduced pressure and dried in a vacuum drier, said catalyst can be obtained.
In other words, the cat

REFERENCES:
patent: 4255283 (1981-03-01), Bartek et al.
patent: 4346020 (1982-08-01), Pretzer et al.
patent: 4484002 (1984-11-01), Lin
patent: 4567307 (1986-01-01), Jones et al.
patent: 4665259 (1987-05-01), Brazdil et al.
patent: 4895987 (1990-01-01), Duggan et al.
patent: 5066629 (1991-11-01), Lukey et al.
patent: 5068485 (1991-11-01), Iton et al.
patent: 5068486 (1991-11-01), Han et al.
patent: 5118654 (1992-06-01), Choudhary et al.

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