A method of obtaining a c2-hydrocarbons

 

(57) Abstract:

The inventive original mixture of methane and oxygen in contact with the catalyst, the composition of which corresponds to the following empirical f - Le: where Me strontium or barium; Me - magnesium or calcium; a= 0,6 - 2,0; b= 0,5 - 2,5; c= 7,0 - 8,9; e= 10,6 - 16, and the introduction of the reaction mixture of water vapor in a quantity of 50 - 80 about. % . The process is carried out at 800 - 850C in flow mode at atmospheric pressure and contact time of 0.25 to 1.0. The content of methane and oxygen in the mixture is from 14 to about 40. % and 4 to about 20. % respectively. The yield of ethylene is 14 and 17.6 mol. % with hydrocarbons up to 20 - 24 mol. % (based on missed methane, after condensation of the water content of products in the mixture obtained after the reaction: ethylene 7,7 - 10,5 about. % , ethane 3 to about 5. % . The catalysts are characterized by high stability. 1 C. p. F. - ly, 1 table.

The invention relates to a method for producing ethylene and ethane, predominantly ethylene. Ethylene is the most large the product of modern chemistry, which is based on a significant part of the production of organic chemistry. Currently, the industrial method for producing ethylene is the cracking of light fractions of petroleum refining. In Kant natural gas. Development of method of obtaining2hydrocarbon oxidative conversion of methane is a new direction of catalysis, which is rapidly developing in the last five years. Analysis of literature data on the search for efficient catalysts and process conditions shows that high output WITH2hydrocarbons (>18 mol. % ) are mainly using metacyclophane mixtures diluted with an inert gas, which leads to the production of gas mixtures after reaction with a low concentration of target products [1-5] .

One of the main problems of the creation of this process is to develop a stable catalytic systems, therefore, proposed in many publications catalysts containing compounds of alkaline and legalistically metals, are of no interest from the point of view of practical implementation of the process [1-3,6] . Is not promising and use as additives in the catalyst halide compounds, although this allows to obtain ethylene with high yield (up to 16-30 mol. % ) [7-10] . This is due to the rapid loss of activity haloesters catalysts, corrosion problems in the equipment and contamination halide compounds.

N the positive transformation of methane use as feedstock metacyclophane mixtures on the catalyst with a content of 0.8 to 10 wt. % La media MgO when 800-845aboutAnd the methane content in the initial mixture 64-78% [11] . The maximum yield of ethylene is to 6.8 mol. % catalyst containing 1.0 wt. % La. The disadvantage of this method is the relatively low yield of ethylene and ethane.

The aim of the invention is to increase the yield of ethylene and ethane in the reaction of oxidative combination of methane without diluting the original reaction mixture with an inert gas in order to obtain, after the reaction gas mixture with a high concentration of target products on the catalysts are characterized by high stability.

This goal is achieved by using a catalyst whose composition corresponds to the following empirical formula: LaaMeb'Mec"CdOeor LaaMeb'Mec"Oewhere Me', strontium or barium, MeI- magnesium or calcium; a = 0,6-2,0; b = 0,5-2,5; c = 7,0-8,9; d = 0.1 to 2.5; e = 10,6-16, and the introduction of the reaction mixture of water vapor in the amount of about 50-80. % . Use as diluent water vapor allows to increase the output WITH2hydrocarbons and after separation of the water of condensation to obtain a high concentration of them in the gas mixture after the reaction. The process osushestvlenie methane and oxygen in the mixture to be about 14-40. % and about 4-20. % respectively.

The catalysts can be prepared by mixing or solutions of nitrate salts, or solutions of nitrates of La, and Me and carbonate Me', by steaming them in a boiling water bath and further annealing at 800about4 o'clock

Distinctive features of the proposed method of carrying out the reaction of oxidative combination of methane in relation to the prototype are:

1) the use of the catalyst composition: LaaMeb'Mec"CdOeor LaaMeb'Mec"Oewhere Me', strontium or barium, Me" as magnesium or calcium; a = 0,6-2,0; b = 0,5-2,5; c = 7,0-8,9; d = 0.1 to 2.5; e = 10,6-16;

2) introduction in the original reaction mixture of water vapor in the amount of about 50-80. % ;

3) the methane and oxygen in the mixture to be about 14-40. per cent and 4.5-17,5 about. % respectively.

Distinctive features of the proposed method of carrying out the reaction of oxidative dimerization of methane are new not only in relation to the prototype, but is unknown to the authors of all other sources related to a method for producing ethylene from methane. The invention has a new quality and can be classified as corresponding to the criterion of "significant differences".

Conducting RL. % (based on missed methane and at the same time be obtained after condensation of the high water content of products in the mixture after the reaction: ethylene - 7,7-10,5 about. % , ethane - about 3-5. % . The proposed catalysts are characterized by high stability. Tests for 300 h show that this decrease in activity is observed. Analysis of the initial mixture and the reaction products spend chromatog - graficheskim method.

P R I m e R 1. In the U-shaped quartz reactor with an inner diameter of 3.0 mm was placed 0.5 cm3catalyst composition La1,0Srthe 2.5Ca7,0Cthe 2.5O16with a grain size of 0.5-1 mm, the Reaction mixture was about. % : 25,5 CH4, 4,5 O2, 70 H2O, is passed through the catalyst at 850aboutWith and contact time = 0,5 sec.

P R I m m e R 2. Similar to example 1, but the reaction mixture has a composition, on. % : 24 CH4, 6 O2, 70 H2O.

P R I m e R 3. Similar to example 1, but the reaction mixture has a composition, on. % : 21 CH4, 9 O2, 70 H2O.

P R I m e R 4. Similar to example 1, but the reaction mixture has a composition, on. % : 32,5 CH4, 17,5 O2, 50 H2O.

P R I m e R 5. Similar to example 3, but the process is conducted on the catalyst composition La1,3Sr0,5Ca8,9C0,B>, 6 O2, 80 H2O, and the composition of the catalyst corresponds to the formula: La1,2Sr1,0Ca8,9C1,0O13,2.

P R I m e R 7. Similar to example 1, but as the catalyst used, the sample composition of La1,3Sr0,5Ca8,9O11,3the reaction mixture has a composition: about. % : 40 CH4, 10 O2, 50 H2O, and the process is carried out at the time of contact = 0,2 sec.

P R I m e R 8. Similar to example 3, but the reaction temperature is 800aboutWith, the process is carried out at contact time = = 1.0 in the presence of a catalyst composition: La1,1Sr2,0Cathe 7.5C2,0O15,1.

P R I m e R 9. In the U-shaped quartz reactor with an inner diameter of 3.0 mm was placed 0.5 cm3catalyst composition La1,1Ba2,0Mgthe 7.5C2,0O15,1with a grain size of 1-2 mm, the Reaction mixture was about. % : 22,5 CH4, 7,5 O2, 70 H2O, is passed through the catalyst at 850aboutWith and contact time = 0.25 in C.

P R I m e R 10. Similar to example 2, but the process is carried out in the presence of a catalyst composition La1,1Ba2,0Cathe 7.5C2,0O15,1and contact time = 0,4 sec.

P R I m e R 11. Similar to example 3, but using the catalyst composition La1,0Sr2,52,0Srthe 2.5Ca6,5O12,0the reaction is carried out at a temperature of 800aboutWith and contact time = 1,0 C.

P R I m e p 13. Similar to example 3, but using the catalyst composition Lafor 0.6Srthe 2.5Ca7,2O10,6.

Outside of the intervals of the selected catalyst composition and the reaction mixture indicated in the claims, the purpose of the invention is not achieved. This is confirmed by the examples 14-19.

P R I m e R 14. Similar to example 2, but the composition of the catalyst corresponds to the formula Lafor 0.4Srthe 2.5Ca7,3Cthe 2.5O15,4.

P R I m e R 15. Similar to example 2, but the composition of the catalyst corresponds to the formula La1,3Sra 0.1Ca9,2Ca 0.1O12,4.

P R I m e R 16. Similar to example 1, but the reaction mixture has a composition, on. % : 80 CH4, 20 O2.

P R I m e R 17. Similar to example 1, but the reaction mixture has a composition, on. % : 64 CH4, 16 O2, 20 H2O.

P R I m e R 18. Similar to example 2, but the reaction temperature is 700aboutC.

P R I m e R 19. Similar to example 3, but the contact time is 0.05 with.

The table presents the results of experiment the wordcourse, the concentration of ethylene and ethane in the dry gas mixture after the reaction.

As can be seen from the data given in the table, the proposed method of carrying out the reaction for oxidizing a combination of methane can increase the yield of ethylene to 14-17,6 mol. % , C2hydrocarbons 20-25 mol. % , the ethylene concentration in the gas mixture after the reaction is 7.7 to 10.5. % . The proposed catalysts are characterized by high stability. (56) 1. Moriyama , T., Takasakii N. , Iwamatsu, E. , K. Aika Oxidative dimerization of methane over promoted magnesium oxide catalysts. Important factors // Chem. Lett. - 1986. - P. 1165-1168.

2. Matsuura I. , Doi , T., Utsumi Y. Oxidative coupling of methane over a Li2O-BeO system catalyst // Chem. Lett. - 1987. - P. 1473-1476.

3. Otsuka K. , Komatsu, T. Conversion of methane to aromatic hydrocarbons by combination of catalysts // Chem. Lett. - 1986. - P. 1955-1958.

4. Machida K. , M. Enyo Oxidative dimerization of methane over cerium mixed oxides and its relation with their ionconducting characteristics // J. Chem. Soc. Chem. Commun. - 1987. - P. 1639-1640.01.

5. Matsuura I. , Utsumi Y. , Nakai, M. , Doi, T. Oxidative coupling of methane over lithium-promoted zinc oxide catalyst // Chem. Lett. - 1986. - P. 1981-1984.

6. Suleimanov, A. I. Oxidative dehydrodimerization methane. Thesis A. Suleymanova, I. Kida. chem. Sciences. - Novosibirsk, 1986. - 180 S.

7. Otsuka K. , Liu Q. , Morikawa A. Selective synthesis of ethylene by partial oxidation of methane over LiCl-Sm2O3// J. Chem. Soc. Chem. Commun. - 1986. - P. 586-587.

8. Wang F.-C , Xu, G. Y. Study of catalysts for the reaction of oxidative combination of methane: effect of lithium chloride on the activity of the oxides of transition metals // Cuihua xuebao, J. Catal. (whale. ). - 1988. - V. 9. - P. 214-217.

10. Wang X.-P. , Lin, Q. , Chao Y. , Shen, U.-F. Oxidizing the combination of methane to put on BaCO3the oxides of metals // Cuihua xuebao, J. Catal. (whale. ). - 1988. - V. 9. - P. 423.

11. USSR author's certificate N 1482905, class C 07 C 2/84, 1989.

1. A METHOD OF OBTAINING A C2-HYDROCARBONS by oxidative conversion of methane at elevated temperature in the presence of oxygen and a catalyst containing lanthanum, alkaline earth metal and oxygen, characterized in that the use of a catalyst containing as the alkaline earth metal is strontium or barium and magnesium or calcium and composition of which corresponds to the following empirical formula

LaaMe MeCdOe< / BR>
where Me- strontium or barium;

Me- magnesium or calcium;

a = 0,6 - 2,0

b = 0,5 - 2,5

c = 7,0 - 8,9

e = 10,6 - 16,

and the process is carried out at 800 - 850oIn the presence of water vapor at the following content of components in the reaction mixture, about. % :

Methane 14 - 40

Oxygen 4,5 - 17,5

Water vapor od, the composition of which corresponds to the following empirical formula:

LaaMe MeCdOe< / BR>
where MeMe, a, b, c, e have the indicated values,

d = 0.1 to 2.5.

 

Same patents:

The invention relates to the synthesis of hydrocarbons oxidation catalytic dimerization of methane, more specifically to a method for producing ethylene and ethane

The invention relates to the synthesis of hydrocarbons oxidation catalytic dimerization of methane, more specifically to a method for producing ethylene and ethane

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55 cl, 1 dwg, 7 tbl, 22 ex

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20 cl, 9 tbl, 9 ex

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3 cl, 8 ex

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4 cl, 1 ex, 1 dwg

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1 cl, 5 ex, 5 tbl

FIELD: chemical industry; other industries; methods and devices for conversion of the methane by the plasma-catalytic oxidation.

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EFFECT: the invention ensures stimulation of the increased efficiency of the conversion process of methane into ethylene.

9 cl, 2 ex, 4 dwg, 1 tbl

FIELD: chemistry.

SUBSTANCE: method involves partial burning of a mixture of methane, hydrogen, oxygen and optionally hydrocarbons, which are different from methane in contact with a catalyst, capable of maintaining burning beyond the normal upper flammable limit of fuel, where they react with formation of product, including one or more olefins. In the mixture coming into contact with the above mentioned catalyst, capable of maintaining burning beyond the normal flammable limit of fuel, can be less than 20 molar % (converted to the overall quantity of the hydrocarbons) of those hydrocarbons which are different from methane. In the mixture coming into contact with the catalyst, the volume ratio of hydrogen to oxygen ranges from 5:1 to 1:1 and methane and oxygen are put into the autothermal cracking device in a mixture at hourly average feed rate of more than 70000 h-1.

EFFECT: invention pertains to the method of obtaining olefins from methane.

12 cl, 2 tbl, 2 ex

FIELD: chemistry.

SUBSTANCE: method of obtaining hydrocarbons C2-C3 by high-temperature catalytic oxidizing conversion of methane lies in supply to reactor, into which catalyst is placed, and whose free volume is filled with inert filling, of initial gas mixture, which contains mixture of methane and molecular oxygen, at rate 50000-70000 m/g/h, catalyst includes into its composition ions of alkali metal, manganese, tungsten and silicon oxide with molar ratio M:W:Mn:Si, where M-Na or K or Rb or Cs, equal 1.8-2.2:1:1.9-2.3:89-92, and is characterised by presence in it of tungsten in oxidation degree W6+, manganese oxidation degrees Mn7+, Mn6+, Mn3+, catalyst being obtained by thermal processing at 200°C and further incineration at temperature 795-799°C of initial solid powder-like mixture, consisting of salts and/or oxides of tungsten, manganese, alkali metal and SiO2, taken in said mole ratio in terms per mole of tungsten, manganese, alkali metal and silicon atoms.

EFFECT: increase of target product output, catalyst productivity, simplification of technology of obtaining target products and reduction of expenditures.

11 cl, 1 tbl, 30 ex

FIELD: chemistry.

SUBSTANCE: aqueous suspension containing earth metal salt, powdered metal chloride and powdered transition metal oxide is made; aqueous suspension is made by dispersing in water the earth metal salt chosen from the group including barium and/or calcium and probably strontium or their combination. Water is added in powdered metal chloride, where powdered metal chloride is chosen from the group including Sn, Mg, Na, Li, Ba. Further powdered transition metal oxide is added being titanium oxide, to water; then plastic binder is added to until paste is formed; paste is dried up paste to powder; powder is heated up at raising temperature following preset temperature profile. Heated powder is baked to produce perovskite catalyst. Suspension contains mixed Ba and/or Ca and/or Sr (0.95mole) + TiO2 + metal chloride chosen from the group Sn, Mg, Na, Li, Ba in amount 0.05 mole.

EFFECT: simplified technology of catalyst producing.

19 cl, 14 ex, 2 tbl, 8 dwg

FIELD: chemistry.

SUBSTANCE: invention relates to two versions of a method for synthesis of aromatic compounds, on of which involves: a methanation step involving contact between a hydrogen-containing gas and carbon monoxide and/or carbon dioxide in the presence of a catalyst which causes reaction of hydrogen contained in the gas with carbon monoxide and/or carbon dioxide and conversion of these components to methane and water; and a step for synthesis of an aromatic compound with reaction of lower hydrocarbon with methane obtained at the methanation step in the presence of a catalyst to obtain a gaseous reaction product containing aromatic compounds and hydrogen, where the aromatic compounds are separated from the gaseous reaction products obtained at the aromatic compound synthesis step, and the remaining hydrogen-containing gas is taken to the methanation step. The invention also relates to a method for synthesis of hydrogenated aromatic compounds obtained using methods described above.

EFFECT: possibility of obtaining aromatic compounds through catalytic reaction of lower hydrocarbons.

14 cl, 13 tbl, 3 ex, 2 dwg

FIELD: chemistry.

SUBSTANCE: invention relates to a method of producing acetylene through oxidative pyrolysis of methane in the presence of oxygen and a catalyst, characterised by that the catalyst is heated to 700-1200°C by passing electrical current through it. The catalyst used is a fechral alloy which is thermally treated on air at temperature 900-1100°C. The ratio of methane to oxygen is varied in the range of 5:1-15:1.

EFFECT: high output and selectivity of the process.

2 cl, 17 ex, 1 tbl, 1 dwg

FIELD: chemistry.

SUBSTANCE: invention relates to a method of converting methane to ethylene and ethane via oxidative conversion, characterised by that the catalyst used in this process is a mixture of quartz and phthalocyanine complexes of magnesium, aluminium or manganese, where the method is realised at temperature 700-800°C.

EFFECT: use of said catalysts increases output of the product.

2 cl, 7 tbl, 7 ex, 2 dwg

FIELD: chemistry.

SUBSTANCE: invention relates to a method for chemical processing of mixtures of gaseous C1-C6 hydrocarbons (alkanes) into C2-C3 olefins (ethylene and propylene), involving oxidative condensation of methane and pyrolysis of C2-C6 alkanes, characterised by that oxidative pyrolysis of C2-C6 alkanes is carried out at temperature 450°C-850°C, pressure 1-40 atm and while feeding not more than 15 vol. % oxygen in the presence of oxide catalysts without preliminary splitting of the initial mixture of gaseous C1-C6 hydrocarbons (alkanes) into components and/or separation of methane; oxidative condensation of methane takes place in a stream of methane separated from products of oxidative pyrolysis of C2-C6 alkanes, in the presence of oxide catalysts at temperature 700°C-950°C, pressure 1-10 atm and molar ratio of methane to oxygen ranging from 2:1 to 10:1, wherein extraction of products of oxidative condensation of methane is carried out collectively or partly collectively with extraction of products of oxidative pyrolysis of C2-C6 alkanes, and methane, ethane and C3+ alkanes separated from reaction gases are recycled and redirected to the methane oxidative condensation and C2-C6 alkane pyrolysis steps, respectively.

EFFECT: method ensures high degree of conversion of the starting material, enables to reduce power consumption on extraction of the desired products, and reduces metal consumption of the equipment per unit product.

8 cl, 2 dwg

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