RU2547845C1 - Catalyst, method for production thereof and method of producing synthesis gas - Google Patents

Abstract

FIELD: chemistry.

SUBSTANCE: invention relates to a catalyst for producing synthesis gas during partial oxidation of methane, which is a microspherical support with a deposited active component based on metal oxides, wherein the microspherical support used is aluminium oxide and/or aluminosilicate particles with diameter of 50-160 mcm, and the active component used is an oxide of Co or Ni or Fe or Mn or Cu or Ce or a mixture of oxides NiO, Co₃O₄ and Ce₂O₃, with the following ratio of components, wt %: said active component 2-40, aluminium oxide and/or aluminosilicate - the balance. The invention also relates to a method of producing the catalyst and a method of producing synthesis gas in the presence of the disclosed catalyst.

EFFECT: high specific output of the product, eliminating explosion and ignition hazard, low power consumption, obtaining synthesis gas with H₂/CO ratio in the range of 1,5-2,5, obtaining a by-product - technical nitrogen - with high conversion of methane-containing material.

7 cl, 3 tbl, 13 ex

Description

The invention relates to the field of petrochemistry and the development of a catalyst for producing synthesis gas in the process of partial oxidation of methane.

A known method and catalyst for producing synthesis gas by the method of partial oxidation of methane described in patent RU 2144844, according to which the synthesis gas is obtained by selective catalytic oxidation of methane with oxygen at a temperature of 700-850 ° C. The specified method has the disadvantage that it is necessary to simultaneously feed raw materials (methane) and an oxidizing agent (oxygen) into the reactor, which leads to an increased explosion hazard of the process due to the formation of mixtures of methane with oxygen. Another disadvantage of this method is the high cost of producing oxygen.

A known method of producing synthesis gas, described in patent US 2665199 A, publ. 01/05/1954, class C01B 3/30, C01B 3/44, according to which synthesis gas is obtained from gaseous hydrocarbons in a plant consisting of a reactor and a regenerator in the presence of solid particles of a metal oxide in a fluidized state. In the reactor, the oxidation of hydrocarbons with oxygen contained in the solid particles takes place, in the regenerator, the solid particles are oxidized to metal oxide. The hydrocarbon oxidation reaction is carried out in a fluidized bed having the following disadvantages:

- uneven residence time of the raw materials in the reaction zone, as a result, some of the raw materials are subjected to excessive conversion to the formation of soot, and the other part does not achieve complete conversion;

- the average fictitious residence time of the raw material in the reaction zone is not small enough to provide the highest selectivity of the process.

As metal oxide, iron oxide is used. The use of metal oxide without a carrier can lead to sintering or agglomeration of particles. To prevent agglomeration and to ensure a high contact area of the active phase and the reagents, application of the active component of the catalyst to any inactive or inert material is used [J. Anderson. The structure of metal catalysts. / M .: Mir, 1978].

Closest to the claimed technical essence and the achieved effect are a catalyst and a method for producing synthesis gas described in US patent 6833013 B1, publ. 12/21/2004, class C01B 3/32, according to which synthesis gas is produced by partial oxidation of lower alkanes with oxygen contained in solid particles containing metal oxide and undergoing redox cycles. Lower alkanes are oxidized in the reactor at a temperature of 800-1100 ° C and a pressure of 0.5-5 MPa, solid particles are oxidized in the regenerator at a temperature of 750-1050 ° C. The resulting synthesis gas contains 60.2% H ₂ and 30.6% CO, i.e. the molar ratio of H ₂ / CO in it is 1.97, which is well suited for the production of methanol from the synthesis gas, Fischer-Tropsch synthesis products. According to an example, in the described method for producing synthesis gas, the catalyst contains 20 wt.% Chromium oxide (VI). During the reaction with hydrocarbons to form hydrogen and carbon monoxide, chromium (VI) oxide is reduced to chromium (III) oxide. Thus, chromium oxide (VI) acts as a donor of "active oxygen" involved in the partial oxidation of hydrocarbons. The effectiveness of the described method for producing synthesis gas depends on its content in the catalyst: the more active oxygen the catalyst can store, the more raw materials can be converted in its presence. Based on the data presented in this patent, the content of active oxygen on the oxide-chromium catalyst is 4.8 wt. %

However, the disadvantage of the described method is the use of a catalyst based on chromium oxide. Chromium and its compounds are toxic substances [Plyushchev V.E. Handbook of rare metals / M .: Mir, 1978], therefore, the use of the proposed method for producing synthesis gas significantly increases the requirements for the level of safety and environmental protection. Another disadvantage of the described method is the reaction of hydrocarbon oxidation and solid particle regeneration in the fluidized bed, which results in a very low specific removal of the product, namely 0.159 kg of synthesis gas per kilogram of catalyst per hour, which negatively affects the performance of the reactor. Specific removal refers to the amount of product obtained by carrying out the process on a catalyst of a certain mass per unit time [Melnikov E.Ya. Reference book of nitrogen. / M .: Chemistry, 1967, 492 C.]. The specific removal of the product in the closest analogue was calculated based on the amount of catalyst in the reactor - 1400 g and the product yield - 516 l / h.

The objective of the present invention is to create an oxide-metal catalyst for producing synthesis gas by partial oxidation of methane free of chromium and its compounds and capable of multiple redox transitions, as well as to increase the specific removal of the product while maintaining the advantages of the closest analogue - eliminating the formation explosive mixtures and low energy consumption with the possibility of producing synthesis gas with a ratio of N ₂ / CO in the range of 1.5-2.5.

The solution to this problem is achieved by the fact that the synthesis gas catalyst in the process of partial methane oxidation is a microspherical carrier, which is used as particles with a diameter of 50 to 160 μm aluminum oxide and / or aluminosilicate, and Co as the active component, or Ni, or Fe, or Mn, or Cu, or Ce, or a mixture of oxides NiO, Co ₃ O ₄ and Ce ₂ O ₃ , in the following ratio of components,% wt:

specified active component 2-40 alumina and / or aluminosilicate  rest

The catalyst is obtained by applying the precursor of the active component - solutions of salts of these metals - on a microspherical carrier with a particle diameter of from 50 to 160 microns by impregnation by moisture absorption, drying at a temperature of from 90 to 120 ° C for 1-5 hours and calcining at a temperature of from 500 to 1200 ° C for 2-8 hours.

The synthesis gas is obtained by oxidizing the conversion of methane-containing gas at a temperature of more than 750 ° C in a reactor using a catalyst as an oxidizing agent — a microspherical support coated with an active component based on metal oxides — and regenerating the reduced catalyst by oxidizing it in a regenerator, from which the regenerated catalyst enters a reactor, wherein said catalyst is used, oxidative conversion is carried out in a through-flow elevator reactor through which the catalyst is continuously It extends upward across a methane-containing gas stream with a residence time of raw materials in the reaction zone of 0.1-10 seconds, and then discharged from the reactor the recovered catalyst separated from the product - the synthesis gas - and sent to the regenerator.

The oxidative conversion is preferably carried out at a temperature of from more than 750 to 1100 ° C, most preferably 850 ° C.

The regeneration of the catalyst is preferably carried out in a fluidized or forced fluidized or semi-through stream by oxidation with an oxygen-containing agent.

As the oxygen-containing agent, air or oxygen is preferably used.

It is generally accepted that the fluidized bed is present at gas flow rates of up to 0.8 m / s. At gas speeds of 0.8-1.5 m / s, the system is characterized by the state of a forced fluidized bed. Systems in which the movement of solid particles is carried out at gas velocities reaching 1.5-3.0 m / s are called semi-through flow. Gas flow rates above 3-4 m / s correspond to the movement of solid particles in the gas stream in the through flow mode [S. Hadzhiev Cracking of oil fractions on zeolite-containing catalysts / M.: Chemistry, 1982. - 280 C.].

Reactors operating in the last two modes are called flow-through (elevator reactors).

The process is continuous, and it is carried out in two spatially separated apparatuses: a reactor and a regenerator. In such a reactor-regenerator system, the catalyst is removed from the system in the form of dust as it is abraded and destroyed, and replaced with fresh.

The resulting synthesis gas and the recovered catalyst are removed from the reactor and the spent (recovered) catalyst stream is separated from the target product stream. The stream of reduced catalyst through a transport line is fed to a regeneration unit, where the catalyst is oxidized in a stream of an oxygen-containing agent (air, oxygen). The catalyst is then separated from the regeneration gases and fed back to the conversion reactor via transport lines, as described above.

The process is continuous and consists of the following stages:

- the conversion of hydrocarbons into synthesis gas (with the restoration of the catalyst to a metallic state);

- catalyst regeneration (with oxidation of its metal components).

The stages of oxidation and reduction of the catalyst are parallel and continuous.

Thus, the catalyst is continuously circulated, and oxygen is transferred from the regeneration zone to the reaction zone, and the material and thermal balances are reduced.

As the catalyst carrier, microspherical alumina and / or aluminosilicate are used. The particle diameter of the carrier is from 50 to 160 μm, the specific surface area is from 10 to 330 m ² / g.

The technical result achieved is:

- to increase the specific removal of the product;

- the possibility of using hydrocarbon raw materials containing carbon dioxide;

- to reduce the risk of explosion and fire, low energy consumption, obtaining synthesis gas with a ratio of H ₂ / CO in the range of 1.5-2.5.

- in the use of catalysts containing less toxic substances than chromium compounds;

- the possibility of obtaining a by-product of technical nitrogen.

The essence of the invention is illustrated by the following examples.

Example 1

A microspherical aluminosilicate carrier is prepared by mixing aqueous suspensions of sodium silicate and aluminum sulfate in such proportions that the aluminosilicate composition has a composition of Na ₂ O (Al ₂ O ₃ · nSiO ₂ ), where n is a molar ratio of SiO ₂ / Al ₂ O ₃ and equal to 2 , 3, followed by obtaining a microspherical form by spray drying and calcining at 800 ° C for 3 hours. 100 g of a microspherical aluminosilicate carrier are impregnated by moisture absorption in an aqueous solution obtained by mixing 57.9 g of Ni (NO ₃ ) ₂ · 6H ₂ O, 53.9 g Co (NO ₃ ) ₂ · 6H ₂ O, 41.0 g Al (NO ₃ ) ₃ · 9H ₂ O, and 4.7 g Ce (NO ₃ ) ₃ · 6H ₂ O at a temperature of 90 ° C. The sample is dried at a temperature of 100 ° C and then calcined in an oven at a temperature of 500-900 ° C for 3-5 hours. The resulting catalyst contains 10.8 wt. % NiO, 10.8 wt. % Co ₃ O ₄ ,

4.1 wt.% Al ₂ O ₃ , 1.4 wt.% CeO ₂ , the rest (70.2 wt.%) Is an aluminosilicate carrier. The amount of active oxygen in the catalyst is 5.2 wt.%, The diameter of the microspheres is from 50 to 160 microns. The catalyst was tested in the partial oxidation of methane.

Methane is fed to the bottom of the elevator reactor, which is in contact with the microspherical catalyst coming from the regenerator. The catalyst, caught in an upward flow of methane, moves upward through the reactor in the through flow mode, and methane is oxidized by the oxygen contained in the catalyst to carbon monoxide and hydrogen by the reaction

CH ₄ + [O] → CO + 2H _2.

Methane is supplied at such a rate as to maintain a residence time of the feed in the riser reactor of 2.1 s. The temperature in the reaction zone is kept at 850 ° C. The product pairs are separated from the catalyst, and the catalyst is sent to a regenerator. In the regenerator, the catalyst is subjected to air oxidation in a fluidized bed mode. The temperature in the regeneration zone is kept at 600 ° C. The oxidized catalyst from the regenerator is again sent to the lower part of the reactor.

The conversion of raw materials is calculated as the ratio of the amount of converted raw materials to the original, expressed in%:

, $$X=\left(\frac{m_f-m_p}{m_f}\right)\cdot \mathrm{one\; hundred}$$

,

where X is the conversion of raw materials, wt.%,

m _f is the mass of raw materials, kg,

m _p - mass of hydrocarbons in products, kg.

The specific removal of synthesis gas is calculated as the amount of synthesis gas obtained from one kilogram of catalyst per hour:

, $$P=\frac{m_{sg}}{m_{cat}\cdot \tau }$$

,

where P is the specific removal of synthesis gas, kg / (kg cat. · h),

m _sg is the mass of synthesis gas obtained during time τ, l,

m _cat is the mass of the catalyst in the reactor, kg,

τ is the time, s.

The molar ratio of H ₂ / CO is calculated as the ratio of the amount of hydrogen to the amount of carbon monoxide in the reaction products:

. $$N=\frac{n_{H_2}}{n_{CO}}$$

.

The process indicators are shown in table 1.

As can be seen from the table, the specific consumption of synthesis gas increases significantly (compared with the specific consumption of synthesis gas of the prototype - 0.159 kg / (kg cat. · H) with a high value of the conversion of raw materials.

Example 2

The experiment is carried out as in example 1, but the process is carried out at a temperature in the reaction zone of 750 ° C in the presence of a catalyst obtained by moisture absorption of 100 g of microspherical aluminum oxide (obtained by spray drying a suspension of aluminum hydroxide) with an aqueous solution of 88.6 g Fe (NO ₃ ) ₃ · 9H ₂ O, at a temperature of 90 ° C. The catalyst contains 14.5 wt.% Fe ₃ O ₄ , the rest (85.5) alumina carrier.

The conversion of raw materials according to the example is 60.3%.

The specific removal of synthesis gas according to the example is 2.180 kg / (kg cat. · H).

The process indicators are shown in table 1.

Example 3

The experiment is carried out as in example 1, but the temperature in the reaction zone is maintained equal to 950 ° C.

The conversion of raw materials according to the example is 99.4%.

The specific removal of synthesis gas according to the example is 3,649 kg / (kg cat. · H).

The process indicators are shown in table 1.

Example 4

The experiment is carried out as in example 1, but the temperature in the reaction zone is maintained equal to 1000 ° C.

The conversion of raw materials according to the example is 99.6%.

The specific removal of synthesis gas according to the example is 3,649 kg / (kg cat. · H).

The process indicators are shown in table 1.

Example 5

The experiment is carried out as in example 1, but the process is carried out at a temperature in the regeneration zone equal to 800 ° C in the presence of a catalyst containing cobalt oxide deposited on an aluminosilicate carrier obtained by moisture absorption of 100 g of a microspherical aluminosilicate carrier with an aqueous solution of 64.2 g Co (NO ₃ ) ₂ · 6H ₂ O, at a temperature of 90 ° C. The catalyst contains 15.1 wt.% Co ₃ O ₄ , the rest (84.9) aluminosilicate carrier.

The conversion of raw materials according to the example is 95.1%.

The specific removal of synthesis gas according to the example is 3.460 kg / (kg cat. · H).

The process indicators are shown in table 1.

Example 6

The experiment is carried out as in example 5, but the temperature in the regeneration zone is kept equal to 1100 ° C.

The conversion of raw materials according to the example is 95.1%.

The specific removal of synthesis gas according to the example is 3.460 kg / (kg cat. · H).

The process indicators are shown in table 1.

Example 7

The experiment is carried out as in example 1, but the process is carried out at a temperature in the reaction zone of 1100 ° C and a residence time of the raw material in the reaction zone of 0.1 s in the presence of a catalyst obtained by moisture absorption by impregnation of 100 g of microspherical alumina (obtained by spray drying a suspension of aluminum hydroxide) 89.4 g of Ni (NO ₃ ) ₂ · 6H ₂ O, at a temperature of 90 ° C. The catalyst contains 18.7 wt.% NiO, the rest (81.3) alumina carrier.

The conversion of raw materials according to the example is 20.4%.

The specific removal of synthesis gas according to the example is 19.147 kg / (kg cat. · H).

The process indicators are shown in table 1.

Example 8

The experiment is carried out, as in example 7, with a residence time of the raw material in the reaction zone of 5.0 s and a temperature in the reactor of 850 ° C.

The conversion of raw materials according to the example is 99.4%.

The specific removal of synthesis gas according to the example is 1.374 kg / (kg cat. · H).

The process indicators are shown in table 1.

Example 9

The experiment is carried out, as in example 8, with a residence time of the raw material in the reaction zone equal to 10.0 s.

The conversion of raw materials according to the example is 99.2%.

The specific removal of synthesis gas according to the example is 0.711 kg / (kg cat. · H).

The process indicators are shown in table 1.

Example 10

The experiment is carried out as in example 1, but as a methane-containing feed, a gas mixture consisting of methane and ethane with a concentration of the latter of 20 vol% is fed to the elevator reactor, and the catalyst contains manganese oxide supported on an aluminosilicate carrier and obtained by impregnation with moisture absorption of 100 g of a microspherical aluminosilicate carrier with an aqueous solution of 40.3 g of Mn (NO ₃ ) ₂ · 6H ₂ O, at a temperature of 90 ° C. The catalyst contains 10.9 wt.% MnO ₂ , the rest (89.1) is an aluminosilicate carrier.

The conversion of raw materials according to the example is 92.3%.

The specific removal of synthesis gas according to the example is 3.792 kg / (kg cat. · H).

The process indicators are shown in table 1.

Example 11

The experiment is carried out as in example 1, but a reaction gas mixture consisting of methane and carbon dioxide with a concentration of the latter of 10 vol% is fed into the elevator reactor, and the catalyst contains copper oxide deposited on an aluminosilicate carrier and obtained by moisture absorption by 100 g microspherical aluminosilicate carrier with an aqueous solution of 92.3 g Cu (NO ₃ ) ₂ · 6H ₂ O, at a temperature of 90 ° C. The catalyst contains 19.9 wt.% CuO, the rest (80.1) aluminosilicate carrier.

The conversion of raw materials according to the example is 91.6%.

The specific removal of synthesis gas according to the example is 3.436 kg / (kg cat. · H).

The process indicators are shown in table 1.

Example 12

The experiment is carried out as in example 1, but a reaction gas mixture is supplied to the elevator reactor, the composition of which is given in table 2. The composition of this mixture corresponds to the average composition of associated petroleum gases (APG) of Russia and the CIS. Associated gases - gaseous hydrocarbons accompanying crude oil, under reservoir pressure conditions, dissolved in oil and released during its production. Associated gases contain 30-80% methane, 10-26% ethane, 7-22% propane, 4-7% butane and isobutane, 1-3% n-pentane and higher n-alkanes. Also, these gases contain hydrogen sulfide, carbon dioxide, nitrogen, inert gases, mercaptans. The average gas factor of Russian oil fields is 95-112 cubic meters. m / t (the amount of associated gases per cubic meter per 1 ton of extracted oil) To calculate the average composition of the model mixture (concentrations of methane, ethane, propane and butane), we used data on the composition of the associated gas of some oil fields in the Russian Federation and the CIS (table 3 ) [Lapidus A.L., Golubeva I.A., Zhagfarov F.G. Gas chemistry. M .: TsentrLitNefteGaz, 2008].

The concentration of each component in the composition of the model mixture was calculated:

c _cpi = 100 · Σ (c _ij · p _j ) / Σ (Σ (c _ij · p _j ) _i ),

where c _ij is the concentration of the i-th component in the j-th field,

p _j - j-th field.

The catalyst consists of nickel, cobalt and cerium oxides supported on aluminosilicate and alumina.

The conversion of raw materials according to the example is 97.6%.

The specific removal of synthesis gas according to the example is 4.739 kg / (kg cat. · H).

The process indicators are shown in table 1.

The molar ratio of H ₂ / CO in the resulting synthesis gas is 2.1.

The nitrogen concentration in the regeneration gas is 99.1% vol.

As can be seen from table 1, a decrease in the residence time of the raw material in the reaction zone below a certain value (2 s) leads to an increase in product removal, but a decrease in the degree of conversion, which in turn will require separation of unreacted raw materials from the reaction products. An increase in the residence time of the raw material in the reaction zone up to 10 s is associated with a decrease in the flow rate, which can lead to a transition of the reactor operation mode from a through flow to a half-through flow and, accordingly, a decrease in product removal.

When the reaction temperature decreases to 750 ° C, the conversion and removal of the product decreases.

Thus, the proposed method for producing synthesis gas, which allows under optimal conditions at high values of the conversion of methane-containing raw materials to increase the specific removal of synthesis gas by 20-30 times compared with the prototype when the ratio of H ₂ / CO in the range of 1.5-2.5 , with the exception of the danger of explosion and fire and low energy consumption.

Example 13

The experiment is carried out, as in example 1, but the catalyst in the regenerator is oxidized with oxygen.

The conversion of raw materials according to the example is 95.1%.

The specific removal of synthesis gas according to the example is 3.460 kg / (kg cat. · H).

The process indicators are shown in table 1.

Table 1 Conditions and Results No. pr. Source components The composition of the catalyst, wt.% The diameter of the catalyst particles, microns Temperature in the reactor, ° C Temperature in the regenerator, ° C The residence time of the reaction mixture in the elevator reactor, s Specific removal of synthesis gas, kg / (kg cat. · H) The conversion of raw materials, wt.% H ₂ / CO, mol / mol The concentration of N ₂ in the regeneration products,% vol. one CH ₄ 10.8% NiO + 10.8% Co ₃ O ₄ + 1.4% Ce ₂ O ₃ + 4.1% Al ₂ O ₃ + 72.9% ACH * 50-160 850 600 2.1 3,460 95.1 2.1 99.1 2 CH ₄ 14.5% Fe ₃ O ₄ + 85.5% Al ₂ O ₃ 50-160 750 600 2,3 2,180 60.3 2.2 99.0 3 CH ₄ 10.8% NiO + 10.8% Co ₃ O ₄ + 1.4% Ce ₂ O ₃ + 4.1% Al ₂ O ₃ + 72.9% ACH 50-160 950 600 1.9 3,649 99,4 2.2 99.3 four CH ₄ 10.8% NiO + 10.8% Co ₃ O ₄ + 1.4% Ce ₂ O ₃ + 4.1% Al ₂ O ₃ + 72.9% ACH 50-160 1000 600 1.8 3,649 99.6 2.2 99.1 5 CH ₄ 15.1% Co ₃ O ₄ + 84.9% ACH 50-160 850 800 2.1 3,460 95.1 2.1 99.1 6 CH ₄ 15.1% Co ₃ O ₄ + 84.9% ACH 50-160 850 1100 2.1 3,460 95.1 2.1 99,2 7 CH ₄ 18.7% NiO + 81.3% Al ₂ O ₃ 50-160 1100 600 0.1 19,147 20,4 2.2 99.1 8 CH ₄ 18.7% NiO + 81.3% Al ₂ O ₃ 50-160 850 600 5,0 1,374 99,4 2.2 99,2 9 CH ₄ 18.7% NiO + 81.3% Al ₂ O ₃ 50-160 850 600 10.0 0.711 99,2 2.2 99.3 10 CH ₄ + 20% C ₂ H ₆ 10.9% MnO ₂ + 89.1% ACH 50-160 850 600 2.1 3,792 92.3 1.8 99.0 eleven CH ₄ + 10% CO ₂ 19.9% CuO + 80.1% ACH 50-160 850 600 2.1 3,436 91.6 1.8 99.0 12 PNG 10.8% NiO + 10.8% Co ₃ O ₄ + 1.4% Ce ₂ O ₃ + 4.1% Al ₂ O ₃ + 72.9% ACH 50-160 850 600 2.1 4,739 97.6 1.7 99.1 13 CH ₄ 10.8% NiO + 10.8% Co ₃ O ₄ + 1.4% Ce ₂ O ₃ + 4.1% Al ₂ O ₃ + 72.9% ACH 50-160 850 600 2.1 3,460 95.1 2.1 0,0 * ACH - microspherical aluminosilicate carrier composition of Na ₂ O (Al ₂ O ₃ · nSiO ₂ )

table 2 The average composition of associated petroleum gases (APG) Gas component CH ₄ C ₂ H ₆ C ₃ H ₈ C ₄ H ₁₀ Concentration, vol.% 70 12 12 6

Table 3 Composition of oil associated gases of some oil fields in Russia and the CIS Field Oil reserves, million tons Component,% vol. CH ₄ C ₂ H ₆ C ₃ H ₈ C ₄ H ₁₀ Samotlor, Zap. Siberia 3200 82.88 4.23 6.48 3,54 Varyogansk 66 77.25 6.95 9.42 4.25 Pravdinskoe 1800 58.40 11.65 14.53 9.20 South Balyk 200 68.16 9.43 15.98 4,50 Romashkinskoye, Tatarstan 2700 43.41 20.38 16.23 6.39 Kuleshovskoe, Samarsk. reg. 60 39.91 23.32 17.72 5.78 Korobkovskoye, Volga. reg. 90 76.25 8.13 8.96 3,54 Yarinskoye Perm. 80 23.90 24.90 23.10 13.90 Kamennolozhskiy Perm 80 28.90 25.90 20.30 9.30 Gnedintsevskoe, Ukraine 38 5.50 27.39 38.35 12.82 Uzen, Kazakhstan 1100 83.53 8.73 3.98 1.92 Zhetybai, Kazakhstan 330 78.06 8.49 6.32 3.46 Rechitskoe, Belarus 114 51.60 15.74 16.11 9.15

Claims (7)

1. The catalyst for producing synthesis gas in the process of partial oxidation of methane, which is a microspherical carrier coated with an active component based on metal oxides, characterized in that particles with a diameter of 50 to 160 microns of aluminum oxide and / or aluminosilicate are used as microspherical carrier, and as an active component - oxide of Co or Ni, or Fe, or Mn, or Cu, or Ce, or a mixture of oxides NiO, Co ₃ O ₄ and Ce ₂ O ₃ , in the following ratio, wt.%:
specified active component 2-40 alumina and / or aluminosilicate rest 2. A method of producing a catalyst according to claim 1, comprising applying the precursor of the active component — solutions of salts of these metals to a microspherical carrier — alumina and / or aluminosilicate with a particle diameter of from 50 to 160 microns by impregnation by moisture absorption, drying at a temperature of from 90 to 120 ° C for 1-5 hours and calcination at a temperature of from 500 to 1200 ° C for 2-8 hours. 3. A method for producing synthesis gas, including the oxidative conversion of a methane-containing gas at a temperature of more than 750 ° C in a reactor using a catalyst as a oxidizing agent — a microspherical support coated with an active component based on metal oxides — and regenerating the reduced catalyst by oxidizing it in a regenerator, from which regenerated catalyst enters the reactor, characterized in that the catalyst according to claim 1 is used, the oxidative conversion is carried out in a through-flow elevator reactor, through which the catalyst continuously passes from bottom to top in a methane-containing gas stream during a residence time of 0.1-10 s in the reaction zone, then the reduced catalyst coming out of the reactor is separated from the product — synthesis gas — and sent to the regenerator. 4. The method according to p. 3, characterized in that the oxidative conversion is carried out at a temperature of from more than 750 to 1100 ° C. 5. The method according to p. 4, characterized in that the oxidative conversion is carried out at a temperature of 850 ° C. 6. The method according to one of paragraphs. 3-5, characterized in that the regeneration of the catalyst is carried out in a fluidized, or forced fluidized, or half-through stream by oxidation with an oxygen-containing agent. 7. The method according to p. 6, characterized in that oxygen or air is used as the oxygen-containing agent.