Catalyst, method of preparation thereof, and a synthesis gas generation method

FIELD: hydrocarbon conversion catalysts.

SUBSTANCE: catalyst for generation of synthesis gas via catalytic conversion of hydrocarbons is a complex composite composed of ceramic matrix and, dispersed throughout the matrix, coarse particles of a material and their aggregates in amounts from 0.5 to 70% by weight. Catalyst comprises system of parallel and/or crossing channels. Dispersed material is selected from rare-earth and transition metal oxides, and mixtures thereof, metals and alloys thereof, period 4 metal carbides, and mixtures thereof, which differ from the matrix in what concerns both composition and structure. Preparation procedure comprises providing homogenous mass containing caking-able ceramic matrix material and material to be dispersed, appropriately shaping the mass, and heat treatment. Material to be dispersed are powders containing metallic aluminum. Homogenous mass is used for impregnation of fibrous and/or woven materials forming on caking system of parallel and/or perpendicularly crossing channels. Before heat treatment, shaped mass is preliminarily treated under hydrothermal conditions.

EFFECT: increased resistance of catalyst to thermal impacts with sufficiently high specific surface and activity retained.

4 cl, 1 tbl, 8 ex

 

The invention relates to a process for production of synthesis gas by catalytic conversion of hydrocarbons in the presence of oxygen-containing gases and/or water vapor at low contact times and to catalysts for this process.

Synthesis gas (mixture of hydrogen and carbon monoxide) are widely used in large-scale chemical processes such as the synthesis of ammonia, methanol, higher alcohols and aldehydes, in the Fischer-Tropsch process and other Synthesis gas used as a reducing gas in ferrous and nonferrous metallurgy, metal working, use environmental settings for neutralization of gas emissions. Perspectivnymi and rapidly developing new areas of utilization of synthesis gas and derived from it are hydrogen vehicles and small energy. Automotive synthesis gas or hydrogen may be used as a Supplement to the main fuel in internal combustion engines or as fuel for an engine based on fuel cells. Energy synthesis gas and hydrogen can be used in combination with fuel cells or gas turbines for the production of environmentally friendly heat and power.

The traditional way to produce synthesis gas is an endothermic process steam reforming of natural gas Nickel catalysts [J.R.Rostrup-Nielsen, Productionof synthesis gas, Catalysis Today, 1993, v.18, 305-324; Usanational, Ovilo // Oxidative conversion of methane. Moscow, Nauka, 1998]. This process is characterized by extremely high capital costs, high operating costs and significant emissions of nitrogen oxides when the flare heating a tubular reformer.

An alternative way to produce synthesis gas - selective catalytic oxidation of hydrocarbons with oxygen (RMS) [S.C.Tsang, J.B.Claridge and M.L.H.Green, Recent advances in the conversion of methane to synthesis gas, Catalysis Today, 1995, V.23 supported, 3-15]. In contrast to steam reforming of natural gas RMS has greater selectivity, is an exothermic process and proceeds effectively at low contact times, thereby enabling it in autothermal mode and reduce the size of the reactor [D.A.Hickman, L.D.Schmidt, Synthesis gas formation by direct oxidation of methane in Catalytic Selective Oxidation", ACS Symposium series, 1993, p.416-426; P.M.Torniainen, X.Chu and L.D.Schmidt, Comparison of monolith-supported metals for the direct oxidation of methane to syngas, J.CataL, 1994, v.146, 1-10] and thereby reduce as energy consumption and capital investment.

The selectivity of the reaction RMSE for target products (carbon monoxide and hydrogen) depends on various factors, but the most important is the chemical composition of the active component. To obtain maximum yields of the target product is synthesis gas, the catalyst should contain the active ingredient, providing high quality, the th activity and selectivity at low contact times in the reaction conversion and the standard deviation of hydrocarbons. In addition, for the implementation of this process requires catalysts with low hydraulic resistance, resistant to thermal shocks and superusuario.

The known method RMSE of methane to produce synthesis gas [U.S. Pat. US 5149464, 01 3/26, 1992] at a temperature of 650-900°C and flow rate 40000-80000 h-1(0,05-0,09 sec) in the presence of a catalyst comprising a transition metal or its oxide, deposited on a thermally stable oxide of one of the elements (M): Mg, B, Al, Ln, Ga, Si, Ti, Zr, Hf, or perovskite-like mixed oxides of General formula MxM'yOz with pyrochlore structure, where M' is a transition metal, including elements in 8 groups. The atomic ratio of the element 8 to the sum of the base elements in these compounds is 1:1 or 3:1, and the noble metal content is 32,9-48 wt.%. The conversion of methane in the presence of mixed oxides Pr2EN2O7, Eu2Ir2O7La2MgPtO6when flow rate 40000 h-1and 777°C is less than 94%, and the increase in flow rate up to 80000 hours-1reduce the conversion of methane to 73% and the selectivity for CO and hydrogen to 82 and 90%, respectively.

In the patent [EP 303438, 01 3/38, 15.02.1989] to obtain a mixture of hydrogen and carbon monoxide offer a way SKO hydrocarbons upon contact of the reaction mixture containing the hydrocarbon, oxygen or oxygen is aderrasi gas and optionally water vapor, with the catalyst in the zone selective catalytic oxidation. Area SKO block contains the catalyst with the ratio of geometric surface/volume is not less than 5 cm2/cm3. The catalyst may contain noble metals, Nickel, cobalt, chromium, cerium, lanthanum and the mixture is deposited on a heat-resistant oxide media, including cordierite, mullite, aluminum titanate, Zirconia spinel, alumina. At the same time, in the patent EP 303438 argue that the speed of reaction of partial oxidation is limited by the rate of mass transfer and does not depend on the chemical nature of the catalyst, which allows in this case to use materials does not exhibit catalytic activity, but providing the necessary ratio of geometric surface/volume. The process is carried out at temperatures in the range 760-1090°and volume rate of from 20000 to 500000 h-1.

In patents [EN 2115617, 01 3/38, 20.07.98; EN 2136581, C 01 B 3/38, 10.09.99; EN 2137702, C 01 B 3/38, 20.09.99; EN 2123471, C 01 B 3/38, 20.12.98; US 5486313, C 07 C 1/02, 23.01.1996 and US 5639401, C 07 C 1/02, 17.06.97] offer a way SKO hydrocarbons, including serosoderjaschei (0.05-100 ppm) [EN 2132299, C 01 B 3/38, 27.06.99; US 5720901, C 07 C 1/02, 24.04.98], in the synthesis gas using catalysts containing precious metals (up to 10 wt.% Pt, Pd, Rh, Os), deposited on a heat-resistant carrier. As carriers are used, for example, α-Al2About32, thermally stabilized oxides of elements of groups III or P And the Periodic table (porous blocks in the form of foam ceramics, resistant to thermal shocks). The process is carried out in the reactor nepodvizhnom layer of catalyst having greater tortuosity is the ratio of the path length of the gas passing through the unit to its length is in the range 1.1-10 at temperatures 950-1300°and flow rate of the gas mixture 2 to 104-108l/kg·the hour. The disadvantages of this method are the large hydraulic resistance of the catalyst layer with high tortuosity and high cost of the catalysts due to the high content of noble metals and used as media of expensive foam ceramics based on zirconium, limiting their practical application.

Thus, the literature describes catalysts based on a block of ceramic substrates with different composition of the active component for the process of selective oxidation of hydrocarbons into synthesis gas at low contact times. Basically, it's the media, representing Panoramico, however, such blocks at low contact times of the reaction mixture have a large hydraulic resistance due to high sinuosity channels. By increasing the size of the macropores to reduce the Hydra is placestogo resistance decreases the mechanical strength and the efficiency of such catalysts by reducing the geometric surface.

It is known that the use of blocks with direct channels (cell blocks) allows to reduce the hydraulic resistance. In the patent [US 5648582, C 07 C 004/02, 30.11.1995] for the process SKO hydrocarbons at space velocities of 800000-12000000 h-1use Pt, Rh or Ni deposited on non-porous ceramic blocks with straight channels. However, these catalysts contain up to 10 wt.% noble metals are very expensive, in addition observed ablation of metals because of the high temperatures developing in the block layer of the catalyst.

The usual lack of catalysts based on non-porous cellular carriers is their low specific surface area [GB 1375830, B 01 J 11/06, 1973; U.S. Pat. EP 0197681, B 01 J 37/00, 18.03.1986], which does not provide them with sufficient activity.

To increase the geometric surface of the catalyst to reduce the thickness of the walls of the cell blocks and increase the number of channels per unit of cross-section of the block. To increase the total surface of the cell carriers in addition put a porous substrate with a high surface area of the oxides of aluminum, silicon, rare earth elements. The latter technique requires special preparation of the materials of construction for the substrate, the introduction of additional stages in the process of manufacture of catalysts [US 3824196, B 01 J 11/06, 16.07.1974]. In addition, because different is the differences of coefficients of thermal expansion may exfoliation of the porous layer during thermal shock, that is typical for any exothermic catalytic processes. Catalysts prepared on the basis of these media have a scarce resource, less resistant to catalytic poisons.

A fundamentally different approach is focused on the manufacture of the monolithic honeycomb catalyst having a high specific surface area and containing the active ingredient directly into the cell structure. In applications [WO 0134517, 01 3/40, 17.05.2001; WO 0160740, 23.08.2001; WO 0160515, B 01 J 37/00, 23.08.2001; WO 0160742, C 01 B 3/40, 23.08.2001] the synthesis gas is produced upon contact of the reaction mixture containing the hydrocarbon, C1-C5and oxygen-containing gas with a catalyst mainly in the form of blocks of foam ceramics based on oxides of transition metals (Cr, Co, Ni, Mn), alkaline earth and rare earth elements with a specific surface area 5-250 m2. The proposed catalysts are not destroyed at a temperature of ~1120-1160°With, however, have a high ignition temperature of the reaction. In addition, the blocks in the form of foam ceramics, as mentioned above, have a large hydraulic resistance.

Known cell block media with high surface area aluminum oxide [US 4294806, B 01 D 53/36, 13.10.1981] or a mixture of aluminum oxide and silicon [U.S. Pat. RF 2093249, B 01 D 53/06, 22.12.1992]. However, such carriers have insufficient mechanical strength and resistance to thermo the Aram. It is not possible to use these media for the manufacture of catalysts for fuel combustion or partial oxidation of methane into synthesis gas, requiring thermal stability at higher temperatures.

To improve thermal stability of the catalyst [US 4637995, B 01 J 23/75, 20.01.1987] use cell block containing 50-90 wt.% sintered ceramic matrix material and 10-50 wt.% material with a high specific surface, dispersed throughout the matrix. Material ceramic matrix consisted of cordierite, mullite, alpha-alumina, or mixtures thereof. The particle size of the matrix material does not exceed 70 μm (200 mesh). Dispersed material had a specific surface area of not less than 40 m2/g and a crystallite size of not more than 0.5 μm and consisted of sulphides of transition metals or mixtures thereof, porous oxides on the basis of aluminum oxide, Zirconia, spinel-based aluminate magnesium, silica, zeolite, titanium oxide or their mixtures, and their mixtures with sulfides of metals.

A disadvantage of the known catalysts and carriers is the use of silicon-containing compounds, which significantly reduce the stability of the monoliths to sintering due to the relatively low melting point compared to aluminum oxide [Quick reference chemist, L.: Chemistry, 1978]. Sulfides of metals at high temperature specification is assured oxidized, that significantly reduces the strength of the contact between particles. For many processes occurring at high temperatures, the reaction is carried out in the diffusion region, it is therefore very high specific surface area is not required. Much more important that the data of the catalyst were resistant to thermal shocks and, if possible, had the high conductivity to reduce the possibility of local overheating. Such properties are composite materials.

Closest to the claimed technical essence and the achieved effect is a block cell catalyst to produce synthesis gas by selective catalytic oxidation of hydrocarbons on the basis of mixed oxides with perovskite structure M1B1-yMyOzand/or fluorite M

1
x
M
2
1-x
Ozwhere M - 8 group (Pt, Rh, Ir), M1a rare - earth element (La, CE, Nd) or alkaline earth (CA, Sr), M2element IV b group (Zr, Hf), In - transition elements (Ni, Co), which is a complex composite containing components with a low coefficient of thermal expansion [U.S. Pat. RF 2204434, B 01 J 23/40, 01 is 3/26, 20.05.2003]. At a temperature of 600-800°and a contact time of 0.1-0.4 sec reaches a high methane conversion and selectivity to synthesis gas. However, the catalyst is a ceramic composite, in which the active component is not included directly in the matrix, forming a honeycomb structure. In addition, the composite is obtained by extrusion, resulting in mechanical stresses and to reduce thermal and mechanical stability of the catalyst.

The invention solves the problem of creating a stable porous block catalyst honeycomb structure having a sufficiently high specific and geometric surface, resistant to local overheating and thermal shock to produce synthesis gas, effective at low contact times as in the reaction of selective catalytic oxidation of hydrocarbons with oxygen and steam and carbon dioxide reforming of hydrocarbons, and a process for production of synthesis gas using the catalyst.

The task is solved by a catalyst for production of synthesis gas by catalytic conversion of a mixture containing a hydrocarbon or mixture of hydrocarbons and oxygen-containing component, which is a complex composite containing alumina and the oxides of rare earth and/or transition metal complex is a composite slabs, the second matrix material, consisting of coarse particles or aggregates of particles dispersed throughout the matrix, and the catalyst has a system of parallel and/or intersecting channels, the dispersed material is a metal oxide, and/or mixtures thereof, and/or metals, or their alloys, and/or metal carbides, and/or a mixture of the composition and structure than the matrix, the content of the dispersed material is 0.5-70 wt.%. Dispersed material can have a particle size from 1 to 250 μm. The catalyst may have a hole in the middle that is different from the channel size and shape.

The use of a matrix that does not contain low-melting compounds, allows to maintain a high porosity and after overheating. The presence of coarse dispersed material, including metals or metal carbides, reduces mechanical and thermal stress in local overheating by increasing the heat capacity of the composite reinforcing properties of the coarse fraction. System of intersecting channels increases the geometric surface of the catalyst and increases its activity. In addition, for durable fixing of the catalyst in the case you can use a block with a hole in the center with a larger diameter than the cell channels, sufficient to securely fasten obtained is a catalyst in the body.

Features of the structure of the proposed catalyst determine the method of its preparation.

The task is also solved by a method of preparation of the catalyst for production of synthesis gas by catalytic conversion of a mixture containing a hydrocarbon or mixture of hydrocarbons and oxygen-containing component comprising a homogeneous mixture of sintered ceramic material of the matrix and the dispersed material, molding the mass into the desired shape, the heat treatment of the molded mass at a temperature sufficient for sintering of the matrix material, as the material of the ceramic matrix using powders containing aluminum metal, a homogeneous mass of impregnated fibrous and/or fabric materials that form in the body of the monolith during sintering system parallel and/or intersecting channels, before heat treatment of the molded mass in hydrothermal pretreated conditions. As the dispersed material used powdered metal oxides, and/or powdered metals and/or alloys and/or metal carbides, and/or their mixture, the content of dispersed material is 0.5-70 wt.%.

The method of preparation of the catalyst honeycomb structure according to the invention includes:

1) use as mater the Ala for ceramic matrix of aluminum powder or powders on the basis of the oxides or hydroxides of aluminum with the addition of aluminum powder;

2) use as an additional material powder particles of large size 1-250 μm, which perform a reinforcing function, and application of metals and carbides improves thermal properties of the media;

3) obtaining a homogeneous mass by mixing and impregnation of this homogeneous mass of fibrous or textile materials, fade with the heat treatment in the air;

4) download a homogeneous mass with vigorelle materials in the mold, permeable to gaseous substances;

5) processing a homogeneous mass under hydrothermal conditions before calcination in air.

Aluminum powder, interacting with water, is oxidized to form hydroxides, which leads to an increase in the volume of the solid body and samouprave a homogeneous mass in a mechanically stable monolith. When ignition occurs thermal decomposition of the hydroxides of aluminum with the formation of a highly porous matrix of aluminum oxide, and finally oxidized aluminum metal with the formation of elongated oxide particles, which along with Krupnyj particles (1-250 µm) reinforced porous matrix and increase its resistance to thermal shocks. In addition, burnable fibers after heat treatment in air is formed through parallel channels in the body of the monolith with sherokhovatymi walls. Burnable mater the materials after heat treatment in air to form a system of channels.

It should be noted that the method of preparation of the catalyst, including the use of powdered aluminum mixed with poroshkoobraznymi non-volatile components, followed by treatment with water vapor is known [U.S. Pat. RF 2059427, B 01 J 23//75, 06.01.1993; U.S. Pat. RF 21322231, B 01 J 37/02, 14.10.1998]. However, this method does not involve the use of additives, fading in the air. It is not possible to produce a honeycomb structure.

As oxides in the present invention can be used simple and/or mixed oxides of transition and rare earth elements. As metals, alloys and carbides are mainly used metals 4 period. The average particle size of metals, alloys and metal carbides determine from the data on the specific surface and the true density of powders. The average size of aggregates of particles of oxides determined by the method of Coulter. In some cases, the particle size is determined by sieving method. Specific surface area determined by BET method [Apokryphos. The adsorption. Texture, particle size and porosity of the materials. Novosibirsk, Nauka, 1999].

The task is also solved by a method for production of synthesis gas by catalytic conversion of a mixture containing a hydrocarbon or mixture of hydrocarbons and oxygen-containing component using the above catalyst which is a complex composite is, containing aluminum oxide, oxides of rare earth and/or transition metals. Complex composite material is a ceramic matrix material consisting of coarse particles or aggregates of particles dispersed throughout the matrix, and the catalyst includes a system of parallel and/or intersecting channels, the dispersed material is a rare earth oxide and/or transition metals, and/or mixtures thereof, and/or metals, or their alloys, and/or carbides of metals of the 4th period of the Periodic table, and/or a mixture of the composition and structure than the matrix, the content of the dispersed material is 0.5-70 wt.%. Dispersed material can have a particle size from 1 to 250 μm. The catalyst may have a hole in the middle that is different from the channel size and shape.

Process for production of synthesis gas is carried out in a flow reactor in autothermal mode at a temperature of 550-1100°With the variations of time of contact and the composition of the reaction mixture. The reaction mixture containing natural gas or vapors of liquid hydrocarbons, such as octane gasoline, and in some examples, the water vapor in the air before entry into the reactor is heated. At the inlet and outlet of the reactor to prevent heat loss put the blocks of corundum. During start-up and operation of the catalyst temperature control the ru gas inlet to the reactor, the temperature of the catalytic unit at the inlet, the outlet temperature of the unit. The reaction products analyzed chromatographically. The efficiency of the catalyst is characterized by the starting temperature of the reaction, the degree of conversion of methane and the amount of produced synthesis gas, expressed in volume% and characterizing the selectivity to synthesis gas. The composition of the initial reaction mixture and the reaction products analyzed chromatographically.

The invention is illustrated by, but is not limited to the following examples.

Example 1. The aluminum powder is mixed with the dispersed material is a mixed oxide LaNi3+xwith perovskite structure with an average size of aggregates of particles of about 15 μm, but with a wide range of size distribution from 1 to 25 μm. The resulting powder was mixed with a solution of glycerine in water. The obtained suspension moisten a cotton cloth in the form of a tape, on top of which is placed cotton yarn thickness 1 mm parallel to each other and perpendicular to the length of the tape. Then the tape rolled into a cylindrical body, which lay in the molding device and placed in the autoclave. Autoclave molding device steamed, resulting in part of aluminum powder is oxidized, and the powder is grasped in the monolith. After ed is claireware the moulder is dried and calcined to a temperature of at least 1000° With, resulting in the remaining part of the aluminum cookislands, and organic materials burn with the formation of channels. Received the product cell structure has a specific surface of 5 m2/, the Number of parallel channels per unit geometric surface of the end plane is 56 cm-2. The distance between the intersecting channels is 0.5 mm, the content of the dispersed material is 22 wt.%. The resulting catalyst was tested in the reaction of selective oxidation of natural gas into synthesis gas. The activity shown in the table.

Example 2. Similar to example 1. Characterized in that, as the dispersed material used powder CEO2with the structure With double oxide having the average size of aggregates of particles of 7 μm. Received the product cell structure has a specific surface area of 10 m2/, the Number of channels per unit geometric surface of the end plane is 40 cm-2. The distance between the intersecting channels is 5 mm, the content of the dispersed material is 26 wt.%.

Example 3. Similar to example 1. Characterized in that, as the dispersed material used powdered Nickel (fraction of 100-250 μm)and aluminum powder added powdered aluminum hydroxide. The resulting product of the honeycomb is the first structure has a specific surface area of 3 m 2/, the Number of channels per unit geometric surface of the end plane is 40 cm-2. The content of the dispersed material is 0.5 wt.%. The resulting catalyst was tested as in example 1.

Example 4. Similar to example 3. Characterized in that, as the dispersed material used powdered alloy Fe-Cr-Al, having the average particle size of 5 μm. Received the product cell structure has a specific surface. The number of concurrent channels per unit geometric surface of the end plane is 35 cm-2. The content of the dispersed material is 70 wt.%.

Example 5. Similar to example 1. Characterized in that, as the dispersed material used powder of solid solution on the basis of oxides of La, Ce, Zr having an average size of aggregates of particles of 8 μm, and a powder alloy Ni-Cr, having an average particle size of 60 μm. Received the product cell structure has a specific surface area of 12 m2/, the Number of channels per unit geometric surface of the end plane is 230 cm-2. The content of the dispersed material is 26 wt.% solid solution on the basis of oxides of La, Ce, Zr and 9 wt.% alloy Ni-Cr. The resulting catalyst was tested as in example 1.

Example 6. Similar to example 3. Characterized in that the qualities of the dispersed material used TiC powder, having an average particle size of 3 μm. Received the product cell structure has a specific surface area of 2 m2/, the Number of channels per unit geometric surface of the end plane is 40 cm-2. The content of the dispersed material is 20 wt.%. The resulting catalyst was tested as in example 1.

Example 7. Similar to example 5. Characterized in that, as the dispersed material used TiC powder analogously to example 6 and the powder CEO2analogously to example 2. Received the product cell structure has a specific surface area of 9 m2/, the Number of channels per unit geometric surface of the end plane is 40 cm-2. The content of the dispersed material is, wt.%: 12 TiC and 8 SEO2.

Example 8. Similar to example 7. Characterized in that, as the dispersed material optionally use the powdered alloy NiCr having an average particle size of 60 μm. Received the product cell structure has a specific surface area of 4 m2/, the Number of channels per unit geometric surface of the end plane is 230 cm-2. The content of the dispersed material is, wt.%: 12 TiC; 8 SEO2; 6 NiCr.

Monolithic catalysts show high efficiency in the reaction of synthesis gas and h is such resistance to thermal shocks.

Thus, as can be seen from the above examples, the present invention solves a technical problem of resistance to thermal shocks at a sufficiently high specific surface area and catalyst activity.

Table.
ExampleIgnition temperature °The contact time, sec.X methane, %The content of CO+H2,.%
15300.088846
37000.118045
57200.1317835
66700.0855430

1. Catalyst for production of synthesis gas by catalytic conversion of a mixture containing a hydrocarbon or mixture of hydrocarbons and oxygen-containing component, which is a complex composite containing alumina, oxides of rare earth and/or transition metals, characterized in that the complex composite includes a ceramic matrix based on aluminum oxide and the material dispersed throughout the matrix, the dispersed material contains oxides of redkozemel is lnyh and/or transition metals, and/or their mixture, and/or metals, or their alloys, and/or carbides of metals of the 4th period of the Periodic table, and/or their mixture in the form of particles or aggregates of particles with a size of 1-250 μm, when the content of dispersed material of 0.5-70,0 wt.%, when this catalyst has a system of parallel and/or intersecting channels

2. The catalyst according to claim 1, characterized in that it can have a hole in the middle that is different from the channel size and shape.

3. The preparation method of catalyst for production of synthesis gas by catalytic conversion of a mixture containing a hydrocarbon or mixture of hydrocarbons and oxygen-containing component comprising a homogeneous mixture of sintered ceramic material of the matrix and the dispersed material, molding the mass into the desired shape, the heat treatment of the molded mass at a temperature sufficient for sintering of the matrix material, wherein the material of the ceramic matrix use powder containing metallic aluminum or powder-based oxides or hydroxides of aluminum and aluminum metal, a homogeneous mass of impregnated fibrous and/or fabric materials that form in the body of the monolith during sintering system parallel and/or overlapping channels, before heat treatment molded mass pretreated in the guide is termalnych conditions, as the dispersed material used oxides of rare earth and/or transition metals and/or their mixture, and/or metals, or their alloys, and/or carbides of metals of the 4th period of the Periodic table, and/or their mixture in the form of particles or aggregates of particles with a size of 1-250 μm, the content of the dispersed material is 0.5-70,0 wt.%.

4. A method for production of synthesis gas by catalytic conversion of a mixture containing a hydrocarbon or mixture of hydrocarbons and oxygen-containing component, by using a catalyst which is a complex composite containing alumina, oxides of rare earth and/or transition metals, wherein the process is carried out in the presence of a catalyst according to any one of claims 1 to 3.



 

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