The catalytic composition suitable for the method of fischer - tropsch

 

The invention relates to the production of catalytic compositions for the Fischer-Tropsch synthesis. Proposed catalytic composition for the synthesis of essentially linear saturated hydrocarbons from synthesis gas containing cobalt in an amount of 1-50 wt.% and tantalum in an amount of 0.05-5 wt.% inert carrier, and the cobalt and tantalum are present in the form of metal or in the form of oxide, and the method of its receipt. The method of synthesis of essentially linear saturated hydrocarbons from synthesis gas using this composition. The technical result is obtained by catalytic composition has a high selectivity for C2+-hydrocarbons. 3 C. and 10 C.p., 6 table.

The invention relates to catalytic compositions suitable for the reaction of obtaining hydrocarbons through the so-called Fischer-Tropsch synthesis; the invention also relates to a catalytic process for the preparation of hydrocarbons, for which it is used.

More specifically, this invention relates to a new catalytic composition for obtaining hydrocarbons via Fischer-Tropsch synthesis, containing cobalt promoted with tantalum, and this song get vetelino below.

The choice of cobalt as the main component of the active phase due to the fact that it promotes the formation of saturated linear hydrocarbons with high molecular weight, minimizing the formation of oxidized and olefinic compounds, in contrast to the well-known catalytic systems based on iron.

Known literature cites many examples of catalysts based on cobalt, used for the synthesis of paraffin products with different distributions.

Since the early work of Fisher in 1932 (N. N. Storch, N. Golumbic and R. B. Anderson, "The Fischer-Tropsch and Related Synthesis", John Wiley and son. Inc., New York, 1951) - which described the development of the system Co/Th2/MgO deposited on kieselguhr, up to the present time proprietary systems based on cobalt are essentially the following: Co/Mg/Th2on kieselguhr as a carrier (1954, Reinpruessen A. G.), Co/MgO in the bentonite as a carrier (1958, M. W. Kellog), Co/Th/Mg (1959, Rurchemie), Co/Th on silica gel as a carrier (1960 Esso Res. and Eng.), Co/Mg/Zr/diatomaceous earth (1968, SU-A-660324, Zeliinskii INST. ), Co/Ru/diatomaceous earth (1976, US-A-4 008 671 GULF), Co/Zr/SiO2(1980, GB-A-2 073 237, Shell), Co/Ru on Titan as the carrier (1988, US-A-4 738 948 Exxon), Co/Re/REO,K on alumina as the carrier (1988, EP-A-313 375, Statoil), Co/Mo,W/K,Na/SiO2(1991, GB-what about the described in literature, is numerous; however, it can be subdivided into different groups concerning the function of the promoter (C. Jager, R. Espinoza in Catalysis Today 23, 1995, 21-22).

For example, promoters such as K, Na, Mg, Sr, si, Mo, W, and metals of group VIII, essentially increase the activity. Ru, Zr, oxides of rare earths (REO), Ti increase the selectivity for hydrocarbons with high molecular weight. EN, REO, Re, Hf, CE, U, Th help regeneriruemost catalyst.

Among the various promoters ruthenium, alone or together with other elements, is definitely the most widely used.

The recent development of catalytic systems for the synthesis of hydrocarbons has led to the identification of different promoters suitable for binding to cobalt to increase both the activity of these systems from the point of view of the transformation of the reactants, and also the selectivity for linear hydrocarbons with high molecular weight. This development took place mainly in the last twenty years. The increase of crude oil prices in the 70-ies gave encouragement to explore other ways of obtaining liquid fuels and chemicals, among which is the possibility of conversion of synthesis gas to hydrocarbon products with high molecular weight through the Deposit of oxide of carbon with the formation of higher hydrocarbons and oxidized molecules with predominantly linear chain. The reaction proceeds in the presence of a mixture of hydrogen and carbon monoxide with carbon dioxide or without (so-called synthesis gas) at temperatures below 350oC and at pressures between 1 and 100 atmospheres.

A wide range of catalysts and their modifications described in the prior art, and a wide range of operating conditions for the reduction reaction of carbon monoxide with hydrogen allows considerable flexibility in selectivity of products ranging from methane to heavy waxes with alcohols and olefins as by-products. The distribution of products can be explained by the known mechanism of growth obtained by the polymerization kinetics and processed Anderson, Shuetz and Flory (P. Biloen, W. M. H. Sachtler, Advance in Catalysis, v. 30, pages 169-171, Academic Press, New York, 1981; R. B. Anderson, Catalysis, v. IV, P. H. Emmett, ed., Reinhold, New York, 1956). In accordance with this model attempts to limit the range of products to maximize, for example With5-C11-fractions (gasoline range), leads to selectively methane and C2-C4-fraction more than 40%. In addition, the products are essentially paraffins with a linear chain and olefins with a low octane number. The only possible deviation from nature, imposed by the polymerization kinetics of the Fischer who ranks examples are systems, developed by Mobil, which essentially combine the properties of the catalysts of the Fischer-Tropsch process with the shape selectivity of zeolite (US-A-4157338).

The opportunity to maximize selectivity for heavy liquids and waxes (essentially paraffin and without sulfur) provides, on the other hand, many benefits. In particular, it is possible to minimize the selectivity for methane and gas fraction. Subsequent processing (for example, hydrocracking, hydroisomerization) this liquid-solid fractions of paraffinic nature gives high-quality middle distillates, when compared with middle distillates derived from petroleum (J. Ball, Gas. Matters, April 27 1989, pages 1-8). In this context, a typical property of catalysts based on cobalt, to be highly selective in the production of higher paraffins, is definitely beneficial. In addition, the use of catalysts with low activity of conversion of water gas, such as catalysts based on cobalt, implies low selectivity for CO2in contrast to conventional catalyst based on iron.

As for the performance of catalysts based on cobalt, defined as weight2+-hydrocarbons/weight of catalyst/vreoci temperature. However, increasing the operating temperature is not justified by increased productivity for liquid and solid hydrocarbons of high quality, as this may cause a consistent increase in the selectivity for methane and light gases. From an economic point of view is very important, on the contrary, to maximize the performance and at the same time to minimize the selectivity for methane. In other words, it is important to maximize the production of liquid and solid hydrocarbons of high quality (C9+With22+).

In accordance with this important purpose, it is necessary that the catalyst was able to combine high productivity (Prod.C2+with a low selectivity to methane (Sl. CH4).

Currently found a catalytic composition, which is applied in the method of Fischer-Tropsch, makes possible a high selectivity for C2+-hydrocarbons and at the same time low selectivity to methane.

In accordance with this present invention relates to a catalytic composition based on cobalt, which allows the conversion of a mixture of CO and H2known as synthesis gas, with N2and/or CO2and/or light gases (C1-C4or without editornote in C2+between 180 and 330 g2+/kgcat/h, maintaining a low selectivity to methane.

The catalytic composition of the present invention essentially consists of an inert carrier, cobalt in an amount of from 1 to 50 wt.%, preferably from 5 to 35 wt.%, and tantalum in an amount of from 0.05 to 5 wt.%, preferably from 0.1 to 3 wt.%, with the complement to 100 consisting of inert carrier, and cobalt, and tantalum are present in the form of metal or in the form of a derivative.

The percent of cobalt and tantalum are expressed as percentages of the metals.

Cobalt and tantalum may be present in the metallic form or in the form of derivatives, and in the latter case, the preferred form of the oxide.

As for the inert carrier, it is preferably selected from at least one of the oxides, at least one of the following elements: silicon, aluminum, zinc, magnesium, titanium, zirconium, yttrium, tin and their respective mixtures.

An inert carrier, which can be used, does not depend on the crystallographic structure of the above oxides. For example, aluminum oxide can be used in any phase composition, such as,,,

In a preferred variant embodiment, the inert carrier is selected from silicon dioxide,-aluminium oxide-aluminium oxide, titanium dioxide and related compounds, even more preferably of silicon dioxide,-aluminium oxide and related compounds.

The next objective of this invention is a method for the catalytic compositions of the present invention, comprising: a) a first deposition on an inert carrier, preferably selected from silicon dioxide and aluminum oxide, preferably by dry impregnation, cobalt salts; subsequent calcination to obtain the catalytic precursor; subsequent optional recovery and passivation calcined product; (b) deposition on the catalyst precursor thus obtained, derived tantalum, preferably by wet impregnation; subsequent calcination, optionally followed by reduction and passivation.

Cobalt and tantalum can be deposited in accordance with various methods, well known specialist is e; gelation and mechanical mixing.

However, in the case of cobalt, the preferred method of dry impregnation. According to this method, the impregnated material is placed in contact with the solution more or less equal to the pore volume. At stage (a), preferably using aqueous solutions of cobalt salts, such as halides, nitrate, oxalate, the complex formed with lactic acid and lactates, the complex formed with tartaric acid and tartratami, the complex formed with acetylacetonates. In a preferred variant embodiment of the use of nitrate of cobalt.

In the case of tantalum, on the other hand, it is preferably precipitated by any of the impregnation method, preferably by wet impregnation. According to this method, an inert carrier, which was pre-deposited cobalt, completely covered with solution derived tantalum, especially tantalum alcoholate, such as ethoxide, propoxide, isopropoxide, methoxide. In the most preferred embodiment, use atoxic tantalum dissolved in C1-C5-alcohols.

The inert carrier may be used to partially or completely in the first phase. In the latter case, all inert carrier ispolzuyut partially in the first phase and partially in the second stage.

In a preferred embodiment, the method of the present invention includes the above stage (a) and (b) without phase recovery and passivation.

As for the calcination, it is a stage of heating at a temperature between 400 and 750oWith the removal of volatile substances and decomposition derivatives of cobalt and tantalum to oxides. The calcination is carried out in the presence of oxygen, air or other gases containing oxygen.

Before this stage the material may be subjected to drying usually under reduced pressure at a temperature of between 80 and 120oC with inert gas or without. The purpose of this activity is to remove (or strong reduction of possible solvents or water, which material was soaked, and ensures the homogeneity of the dispersion of the active phase.

As for recovery, it is a stage in which the material is treated regenerating agent, preferably hydrogen or gas containing hydrogen. The restoration carried out at a temperature between approximately 250oWith approximately 500oC, preferably from 300 to 450oWith, for a time between 0.5 and 24 hours, at pressures between atmospheric pressure and 40 bar.

That casamerica is usually 10-80oC. for Example, using nitrogen containing 1-2% oxygen with a flow of 2 l/h/gcatstage passivation may have a duration of from 1 to 5 hours at 25oC.

Some of the operational details related to obtaining the above-described catalyst compositions will be more apparent upon receiving the experimental examples below, which, however, do not limit the catalytic composition of the present invention.

Further, this invention relates to a method for producing essentially linear, saturated hydrocarbons from synthesis gas (method of Fischer-Tropsch) in the presence of the above catalyst composition.

Conversion of synthesis gas to hydrocarbons occurs at a pressure typically between 1 and 100 bar, preferably from 10 to 75 bar, at a temperature usually in the range 150-350oWith, preferably 170-300oWith even more preferably 200 to 240VoC. hourly Average volumetric flow rate is usually 100-20000, preferably 400-5000, volumes of synthesis gas to volume of catalyst per hour. The relation of H2/CO in the synthesis gas typically ranges from 1:2 to 5:1, preferably from 1.2:1 to 2.5:1. May also be present other gases, especially CO2.

As Isaza, mainly consisting of methane. Oxidizing agent (oxidant) may be oxygen or air. In the latter case, it is obvious that the mixture of synthesis gas will also contain a significant amount of nitrogen, which may or may not be removed from CO/H2before the reaction, Fischer-Tripsa. The advantage of the reaction of the Fischer-Tropsch process on the mixtures, which is still present nitrogen, is obvious.

The catalyst can be used in the form of a fine powder (about 10-700 μm) or in the form of particles having an equivalent diameter of from 0.7 to 10 mm, respectively, in the presence of a liquid phase (under operating conditions) and the gaseous phase or gas phase. The liquid phase may comprise at least one hydrocarbon having at least 5, preferably at least 15, carbon atoms per molecule. In a preferred embodiment, the liquid phase essentially consists of the same reaction product.

As the only example of the catalysts of this invention can be used in a reactor with a fixed bed, which served continuously a mixture of CO and H2and who works under the following conditions: reaction temperature 200-240oWith; the pressure of the reaction 20 bar; space velocity (GH least 45% of the volume of carbon monoxide (converse. WITH%).

Following these conditions, the catalysts obtained as described in examples 1-11, evaluate using a variety of media. The compositions are summarized in table. 1.

The results of the tests of reactivity shown in the table. 2-4.

Catalysts deposited on SiO2Comparative example 1.

Comparative catalyst A (Co/Ru/SiO2; 14%, And 0.2% EN).

The carrier is silicon dioxide (having a surface area of 520 m2/g, specific pore volume of 0.8 m3/g, average particle diameter 0.5 mm, specific gravity of 0.42 g/ml) impregnated with dry nitrogen impregnation with a solution of Co(NO3)26N20 at pH 2.5 in such quantities to get a percentage, equal to 14 wt.% of the total number. Silicon dioxide impregnated thereby, dried at 120oC for 16 hours, calicivirus 400oC in air for 4 hours, then treated in the stream2when flow rate (GHSV) of 1000 h-1in a tubular reactor at 400oC for 16 hours. The sample recovered so Passepartout in a mixture (1%) O2/(99%)of N2with GHSV 1000 h-1for 2 hours at room temperature.

7,5O, obtained according to the following procedure: precipitation in the form of hydroxide at rn,2 RuCl3xH2O, the subsequent removal of chlorides, re-solubilization in concentrated NGO3and dilution in CH3PINES3in the ratio of 1:250 about/about.

A solution of ruthenium in acetone is added to the sample in such a quantity to obtain 0.2 wt. % EN from the total amount. The suspension is left under stirring for 2 hours and then dried in a vacuum less than 10 mm RT. Art. at the 50oC. Phase calcination in air is carried out at 350oC for 4 hours and then carry out the restoration and passivation in the same way as described above.

Comparative example 2.

Comparative catalyst (Co/Sc/SIO, SIS2; 14%, And 0.2% Sc).

To obtain the catalyst In 10-3M solution of SC(NO3)2acetone is added to 50 g monometallic catalyst Co/SIO, SIS2obtained as described in example 1 in such an amount to obtain a final mass% Sc, equal to 0.2%.

Thus obtained, the slurry is mixed for two hours and then dried in vacuum at 50oC. Sample calicivirus at 350oC for 4 hours in air, the barrel is V 1000 h-1for 2 hours at room temperature.

Example 3. Catalyst C1 (Co/Ta/SiO2; 14% Co, 0.5% Of TA).

0.01 M solution of Ta(EtO)5in ethanol is added to 50 g monometallic catalyst Co/SiO2obtained as described in example 1 in such an amount to obtain a final wt.% tantalum, equal to 0.5%.

The suspension thus obtained, leave to mix for two hours and then dried and vacuum at 50oC.

Sample calicivirus at 350oC for 4 hours in air, restore 400oWith N2for 16 hours with GHSV 1000 h-1and Passepartout (1%) O2/(59%) of N2with GHSV 1000 h-1for 2 hours at room temperature.

Example 3b. The catalyst C2 (Co/Ta/SiO2; 14%, And 0.2% TA).

The catalyst C2 receives the same way as described in example 3.

Example 4. Catalyst D (Co/Ta/SiO2; 14% Co, 0.5% Of TA).

The carrier is silicon dioxide (having a surface area of 520 m2/g, specific pore volume of 0.8 m3/g, average particle diameter 0.5 mm, specific gravity of 0.42 g/ml) impregnated with dry nitrogen impregnation with a solution of Co(NO3)26N20 at pH 2.5 in such quantities to get a percentage, equal to 14 wt.% from the total number is oC in air for 4 hours. 0.01 M solution of Ta(EtO)5in ethanol is added to the monometallic sample Co/SiO2in this volume, to obtain the final wt.% tantalum, equal to 0.5%.

The suspension thus obtained, leave to mix for 2 hours and then dried in vacuum at 50oC.

Phase calcination in air is carried out at 350oC for 4 hours.

The catalyst deposited on TiO2Comparative example 5.

Comparative catalyst E (Co/Ru/TiO2; 12%, And 0.2% EN).

Following the procedure described in example 1, comparative catalyst E get as catalyst A, but with the carrier of TiO2instead of SIO, SIS2. In this case, TiO2has a surface area of 25 m2/g, specific pore volume 0,31 cm3/g and a content of rutile 81%.

Comparative example 6.

Comparative catalyst F
(Co/Sc/TiO2; 12%, And 0.2% Sc).

Catalyst F receives the same way as described for the preparation of the catalyst Century

Example 7. Catalyst G (Co/Ta/TiO2; 12% Co, 0.5% Of TA).

Following the procedure described in example 4, get the G catalyst consisting of a carrier on the basis of titanium dioxide. In this case, TiO2has a surface area of 25 m2/g, the specific volume is isator N (/TA/[Si, Ti]; 15% Co, 0.5% Of TA).

The carrier is silicon dioxide (having a surface area of 480 m2/g, specific pore volume of 0.8 m3/g, a particle diameter of between 75 and 150 μm, the specific gravity of 0.55 g/ml, average pore 35 angstroms), previously dried at 150oC for 8 hours, suspended in the atmosphere of nitrogen in dehydrated n-hexane, 6 ml/g SIO, SIS2. To this suspension is added 0.2 M solution of Ti(i-Pro)4in such numbers, in order to obtain approximately 7,0% Ti; the mixture is left under stirring for 16 hours and then dried in vacuum at a pressure less than 10 mm RT. Art. and at a temperature of 50oC. the Sample thus obtained, calicivirus in nitrogen atmosphere at 400oC for 4 hours and then calicivirus in air at 600oC for an additional 4 hours.

Catalyst N get mixed media thus obtained, and the catalyst consists of 7.1 percent titanium, about 25% of which is in crystalline form (50% rutile, 50% anatase), and its surface area is equal to 440 m2/g, similar to that described in example 4.

The catalysts on a carrier Al2O3
Example 9. Catalyst I (With/TA/A1203; 14% Co, 0.5% Of TA).

Catalyst I get the same way as described in example pore volume of 0.5 m3/g, average porethe particle size of between 20-150 μm, specific weight 0,86 g/ml).

Example 10. Catalyst L (/TA/Al2About3; 12% Co, 0.5% Of TA).

Catalyst L receive the same manner as in example 4 with the carrier, aluminum oxide (crystalline phase 50%and 50%the surface area of 137 m2/g, specific pore volume 0.46 m2/g, average porethe particle size of between 20-120 μm, specific weight 0,69 g/ml).

CATALYTIC TESTS
Example 11. Evaluation of catalytic activity of the catalysts supported on silica.

The catalyst (a, b, C, D in accordance with examples 1-4) receive in particles having a diameter between 0.35 and of 0.85 μm and then diluted with an inert carrier, silicon carbide, having the same particle size as the catalyst, and in a volume ratio of the catalyst/inert carrier, equal to 1: 2. Then diluted so the catalyst was loaded into a tubular reactor and subjected to the activation process in a stream of hydrogen (2000 N/hlcat) and nitrogen (1000 N/hlcat) at a temperature of between 350-400oC and a pressure of 1 bar over-1000 N/hlcatand (5000-15000 N/hlcat), respectively, the system is brought to a pressure of 20 bar and then injected carbon monoxide (116,5-500 N/hlcat) to obtain the volumetric relationship of H2/CO = 2.

The flow rate of nitrogen in the initial phase of the reaction is gradually reduced until complete removal according to the following sequence (lower flow rate refer to tests with GHSV = 500 h-1higher flow rate refer to the GHSV = 1500 h-1(see table.A).

At the end of the initial phase of the reaction temperature adjusted so as to obtain the conversion of carbon monoxide relative to the submitted amount (the converse. WITH%) less than 20% for at least 48 hours, then in the next 48 hours the temperature is gradually increased to achieve minimum conversion WITH 45%, but without exceeding the reaction temperature 240oWith, to minimize the formation of methane and light gaseous fractions (3-C4).

As shown in the table. 2 for comparative catalyst A, to achieve the conversion FROM exceeding the limit of 45%, it is necessary to increase the reaction temperature (from 200 to 240oWith increasing alyansa (from 7.8 to 29,7%), expressed as a percentage related to the total carbon present in the products (%), and there has been a General decrease in the selectivity to higher hydrocarbons (sat. C22+from 15.4 to 3.2%, sat. With9+with 66,9 to 48.8%), expressed in percentage of the total weight of all acquired hydrocarbon fraction (wt.%).

As for the comparative catalyst promoted with scandium, using the total flow rate of 1500 h-1and the reaction temperature 218oTo get average weight capacity hydrocarbons with more than 2 carbon atoms (C2+), is equal to 273 g/kg/h, and the selectivity for C22+of 14.2%. In General, the catalytic properties of the catalyst can be considered as higher than the catalytic properties of the catalyst A.

Catalysts Cl, C2 and D of this invention containing tantalum are similar catalytic test. As shown in the table. 2, when the total volumetric flow rate (GHSV) 1500 h-1and the reaction temperature 220oFor catalysts C1 and C2 obtained according to the same procedure as catalysts a and b are CO conversion 60,3 and 69.3 percent, respectively, of performance against With2+more than 315 g9+-hydrocarbons between 65,6 and 71.3% and, finally, the selectivity for C5+more than 81%.

These characteristics are better than the features obtained with the comparative catalysts a and b, especially for higher capacity, selectively higher hydrocarbons and lower selectively methane and light gaseous fractions (2-C4).

As catalyst D, was synthesized according to the procedure described in example 4, the catalytic characteristics of the system With/That is further enhanced in comparison with the comparative catalysts: conversion FROM 71.0 per cent, the performance in respect of C2+330 g2+/kgcat/h, the selectivity for methane 8.4%, and the selectivity for higher22+the hydrocarbons of 29.1%, the selectivity for C9+-hydrocarbons is 78.4% and, finally, the selectivity for C5+83,5%.

Example 12. Evaluation of catalytic activity of the catalysts supported on titanium.

As shown in the table. 3, and in this case also the comparison between the reference catalysts promoted with ruthenium (cat. E) or scandium (cat. F), and catalyst promoted without intermediate recovery phase and phase passivation (example 3), shows that the storage of low selectivity to methane (the converse. WITH 70.0% of the performance With2+172 g/kgcat/h, C22+32, 9%, SN47,6%).

Example 13. Evaluation of catalytic activity of the catalysts deposited on silicon dioxide/titanium dioxide and aluminum oxide.

The catalytic composition With/TA deposited on other materials such as mixed media, silicon dioxide-titanium dioxide and aluminum oxide, with different phase composition showed an interesting catalytic properties at the temperatures of reaction between 209 and 218oAnd the total volumetric flow rates of 1500 h-1.

As shown in the table. 4, obtained by the conversion are more than 57% (converse. WITH 65,8-57,1%), performance in relation to C2+more than 180 g/kg/h (performance C2+: 183,1-260,1 g/kg/h), selectivity With22+-hydrocarbons higher than 23% (sat. With22+for 23.2-28.3 per cent).

The data table. 5 show the possibility of using synthesis gas diluted with nitrogen.


Claims

1. Catalytic composition for the synthesis of essentially linear saturated hydrocarbons from synthesis gas containing cobalt and other components on an inert carrier, and cobalt, and the other component are present in the form of metal or in the form of hydroxy is the total content of the components, wt.%:
Cobalt - 1-50
Tantalum is 0.05-5
Inert media - Rest
2. The catalytic composition under item 1, characterized in that the cobalt is present in an amount of 5 to 35 wt.% and tantalum in an amount of from 0.1 to 3 wt.%.

3. The catalytic composition under item 1, wherein the inert carrier is selected from at least one of the oxides, at least one of the following elements: silicon, aluminum, zinc, magnesium, titanium, zirconium, yttrium, tin and their respective mixtures.

4. The catalytic composition under item 1, wherein the inert carrier is selected from silicon dioxide,-aluminium oxide-aluminium oxide, titanium dioxide and related compounds.

5. The catalytic composition under item 4, wherein the inert carrier is selected from silicon dioxide,-aluminium oxide and related compounds.

6. The method for the catalytic composition under item 1, which includes: a) a first deposition on an inert carrier cobalt salt, calcining to obtain the catalytic precursor and subsequent optional, recovery and passivation calcined product; b) deposition on italianelena and passivation; characterized in that the connection of the other component is used as a compound of tantalum.

7. The method according to p. 6, wherein the inert carrier is selected from silicon dioxide and aluminum oxide.

8. The method according to p. 6, characterized in that the cobalt salts are precipitated on an inert carrier by way of the dry impregnation.

9. The method according to p. 6, characterized in that the compound of tantalum precipitated by wet impregnation.

10. The method for the synthesis of essentially linear saturated hydrocarbons from synthesis gas consisting of CO and H2that includes the reaction of this mixture in the presence of a catalytic composition at 150-350oC, a pressure of 1-100 bar, a molar ratio of N2/CO in the synthesis gas is from 1:2 to 5:1, wherein the reaction is carried out in the presence of a catalytic composition under item 1.

11. The method according to p. 10, characterized in that the synthesis gas consisting of CO and H2, diluted with nitrogen.

12. The method according to p. 10, wherein the process is carried out at 170-300oC, a pressure of from 10 to 75 bar, a molar ratio of N2/CO in the synthesis gas from 1.2:1 to 2.5:1.

13. The method according to p. 10, wherein the process is carried out at 200-240oC.

 

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