Method of heterogeneous catalytic processing of gas mixture with predominant content of methane

FIELD: petrochemical processes.

SUBSTANCE: natural or associated gas and oxidizing gas are passed in continuous or pulse mode at 200-700°C and pressure 1 to 50 atm through catalyst represented by modified naturally occurring mineral schungite containing 90-95% of carbon constituent including 20 to 90% of nanocarbon forms, 70% of which have open channels, or modified schungite as carrier with metallic cocatalyst incorporated therein in amount up to 2%.

EFFECT: increased productivity of process.

6 cl, 18 ex

 

The invention relates to chemical technology, more specifically, to a method of processing gas mixtures with a predominant content of methane, such as natural gas or associated gas, a modified natural shungite with the aim of obtaining higher hydrocarbons.

The invention can be used in the industrial synthesis of a mixture of liquid alkanes from methane, natural gas, associated gas, carbon monoxide (CO) and in several other applications.

When the description of the invention following terms are used.

Nanotechnology - the technology of objects whose size is of the order of 10-9m (BAS): BDT, 1997. S).

Fullerenes are a form of carbon, which represents a closed surface structure, which includes only five - or six-membered ring of carbon atoms. Fullerenes were discovered in the second half of the 80-ies (H.W. Kroto, J.R. Heath, S.C. O'brien et al. C60. Bakminsterfullerene // Nature. 1985. V.318. P.162) and was first produced in macroscopic quantities arc method in 1990 (Kratchmar W., L.D. Lamb, K. Fostiropoulos, D.R. Huffman Solid C60a new form of carbon // Nature. 1990. V.347. P.354).

Fullerene soot - dispersed product of the combustion of carbon materials, usually of graphite containing fullerenes. Fullerene soot is the main raw material for producing fullerenes.

Nanotubes, nanoarray, neolocality, nano-cones nanocarbon forms in which ructure natural or synthetic carbon material. Characteristic morphology of nanotubes is the presence in their structure one or several cylindrical surfaces with a diameter of more than 1 nm, nested into each other and identical in its structure of graphene planes of the graphite. Nanotubes as a new form of carbon was first described in the work (Iijima S. Helical microtubules of graphitic carbon // Nature. 1991. V.35. P.56). The structure related to the nanotube nano-forms that arise, usually at the arc method of their production as a byproduct, described in a review paper (T.W. Ebbesen, Carbon nanotubes: preparation and properties. Ed. Ebbesen T.W., CRS Press, Boca Raton, 1997, p.139).

Shungite is a metamorphic rock, a mineral containing cryptocrystalline carbon (from 30%to 90%) (BAS): BDT, 1997. S). Typical carbon content of shungite is the most various nanocarbon forms with a relatively narrow channel with a diameter of about 1 nm, the characteristic size of 10-15 nm and a large number graptopetalum layers: short and at the same time thick nanotubes, and neolocality, nano-cones, nonabusive (Zaidenberg A.Z., Rozhkova NX, Kovalevsky, V.V. et. al. Physical Chemical Model of Fullerene-like Shungite Rocks // Mol. Mat. 1996. V.8. P.107).

Getting nanocarbon material from shungite - removing the carbon component of the carbon-containing natural raw materials shungite using the method of selective oxidation, subsequent enrichment of this stood the Commissioner nanocarbon forms and disclosure of their channels.

Modified natural shungite is a chemically modified natural schungite, enriched nanocarbon forms. Described material contains from 90 to 95 wt.% carbon content, part of which, from 70 to 90 wt.%, are nanocarbon forms - multi-layer and single-layer nanotubes, nanoarray, neolocality, nano-cones, and from 20 to 70 wt.% abdominal nanocarbon forms have opened channels.

As the depletion of oil reserves in the world are obvious urgent development of industrial technology of the synthesis of liquid hydrocarbons from other carbon-containing minerals: coal, natural gas, peat, biomass of various types, etc.

The most widespread and technologically developed a method of processing natural gas for the purpose of obtaining a mixture of liquid hydrocarbons is the Fischer-Tropsch synthesis, comprising the first step of the conversion of methane in a mixture of hydrogen and carbon monoxide (synthesis gas), and the second stage is the conversion of this mixture in a mixture of liquid alkanes (C5-C8) (FischerF., Tropsch H. // Ber. 1926. Bd.59. S.830). When carrying out the Fischer-Tropsch synthesis uses a variety of non-carbon heterogeneous catalysts: an oxide catalysts, composite oxide catalysts, solid acid catalysts, zeolite-containing catalysts. The activity to which each of them describes the integrated the release of hydrocarbons at 1 m3synthesis gas, and selectively - content (%) of isoalkanes. The use of the most developed types of oxide catalysts (TiO2, ZrO2CeO2and so on) results in the optimal synthesis conditions for the preparation of hydrocarbons in the amount of 20-50 g/m3the synthesis gas. Detailed comparative review of different types of catalysts as at 1997 made in: A.L. Lapidus, Krylov, A. // USP. 1998. T. No. 11. S. Thus, the synthesis of high-quality gasoline with the use of combined active catalysts of the oxides of aluminum, zirconium and rare earth elements with the addition of ZnO, Cr2O2and CuO occurs at extremely high pressures and temperatures. In this case, it may be made out of hydrocarbons up to 150-160 g/m3. The use of zeolite catalysts (e.g., Co-MgO/NaX) allows to reach exit 180 g/m3. However, the percentage of isoalkanes reaches 50 wt.%. The disadvantage of these catalysts is their gradual deactivation as a result of interaction with synthesis gas, sintering metal particles and coking zeolite matrix. As a result of this and other shortcomings of the cost of gasoline produced using the technology of the Fischer-Tropsch process and its modifications, is about $4000/ton (or $3,2/l), 2 - times more expensive than gasoline prices in the EU.

Along with the improvement of the Fischer-Tropsch synthesis is actively seeking ways of directly converting lower hydrocarbons in the highest. In particular, the classical version of fuel production, i.e. hydrocarbons with a low content of aromatic component is oxidative binding compressed methane gaseous oxygen carrier. As metals, recovering oxides which are effective to convert the methane into higher hydrocarbons in the presence of specially selected promoters (halogen-free, phosphorus compounds, etc. and media, as described, for example, indium, germanium, lead, bismuth (U.S. patent№№444364, 4443645, 4443647, 4443644, 4499323, 4499324).

On the contrary, in the presence of solid acid catalysts for the oxidative condensation of methane is accompanied, as a rule, its aromatization (U.S. patent No. 4433192, 4465893, 6552243). Loaded molybdenum catalyst aluminosilicate molecular sieve type NH4-ZSM-5 also provides an efficient aromatization of methane. The process temperature is 600-800°and pressure - less than 5 ATM.

Unfortunately, the production of fuels and chemicals by methods described in these patents, there has been a significant decline in catalyst activity over time. In addition, as in the Fischer-Tropsch synthesis, the product always contains a considerable quantity is about oxides of carbon, coke and water, and the selectivity of the methods to higher hydrocarbons is quite small.

Selectivity can be improved with the use of compressed gas containing nitric oxide along with methane. This was described in U.S. patent 5406017. The authors used a solid non-acidic catalysts of the type MgO, SiO2, Al2About3La2O3, TiO2and ZrO2with very high stability. The drawback of the process was the use of difficult synthesized nitric oxide, for example, N2O that sharply reduced its profitability.

In U.S. patent 6002059 an efficient parallel synthesis of N2O, however, the method of conversion in General, including the synthesis of ammonia and nitrogen in the presence of an additional source of hydrogen is very difficult. By using a source of oxygen ammonia is then converted to oxide (N2O, which connects the methane and provides the necessary conversion.

Possible way to increase the yield of higher hydrocarbons by oxidative linking methane - up to 70% - is the use of the reactor recycling with continuous removal of ethylene (Cordi E.M. et al., // Appl. Catal. A: Gen. 1997. V.155. P.L1; Mashocki A. Appl. Catal. A 1996. V.146. P.391). Ethylene are either directly derived from stream recycling, or converted into other products, and then separated. So, for example, use the catalysis of the Torah Mn/Na 2or WO4/SiO2at a temperature of 800°converting the methane into ethylene (U.S. patent 6596912). Then there is the ethylene oligomerization products on zeolite catalyst H-ZSM-5 at 275°C. the Total yield of higher hydrocarbons reaches 80%, and the output nah above With4up to 50%.

Part of the above methods allows to achieve very high selectivity of the products, however the problem of sintering of the catalytic particles and the associated reduction with time of the catalytic activity remain. Lifetime, including expensive catalysts, providing a high level of conversion is very low and therefore the cost of production remains high.

The problem of deactivation of the catalyst can be effectively overcome with the use of fulleroid materials as the carrier of the catalytic particles. One of such materials, as proposed in U.S. patent 6653509 is ultrafine fullerensoderzhashchie soot is a product of high-temperature evaporation of a graphite anode in an electric arc and crushed cathode Deposit - treated product of recrystallization of the vaporized graphite, formed at the cathode. As an example of catalytic reactions, implemented with a data carrier of a metal catalyst, appear is eacli hydrogenation of carbon monoxide at low temperature (not more than 300° C) and atmospheric pressure, and the reaction of partial oxidation of methanol.

Related fulleroid material that can be the carrier of the catalyst, are carbon nanotubes that grow in the pore size range of 1-100 μm specially made of porous substrates by introducing into the pores of nano-sized germ growth of nanotubes (U.S. patent 6713519). Conversion in process type of Fischer-Tropsch synthesis has in this case the following parameters: temperature 265°C, a pressure of 16 ATM conversion WITH about 35%, the selectivity to methane is about 30%, specific activity (i.e. the number of moles CO converted per 1 g of metal) 1500-2500. The advantage of this method is that along with the catalytic conversion of methane occurs and the catalytic growth of nanotubes, i.e. the renewal of the carrier metal catalyst. The above method is the prototype of the proposed method.

Obviously the principal novelty of the technologies described in the last two mentioned patents, fulleroid products arc synthesis is very expensive and unmanaged growth process of nanotubes in the pores is able by itself to absorb over time, the metal catalyst and inhibit the conversion process.

In the experiments described in: W. Qian, T. Liu, F. Wei, Z. Wang // Carbon. 2003. V.41. P.846), nanosized particles of metal catalyst (Fe the Mo) were placed on the tips of the nanoparticles or their inner surfaces. We investigated the reaction of obtaining pure hydrogen from natural gas by non-oxidative catalytic decomposition of methane. Growth was observed methane conversion with increasing temperature, and the degree of conversion was close to thermodynamic value. Decontamination of Nickel catalysts observed at almost all of the above catalysts have not been reported. The process efficiency was increased due to the additional formation of nanotubes by decomposition of methane. The high cost of artificial nanocarbon material is not possible in this case to go beyond laboratory research.

Thus, given the above, it can be argued that currently, the development of highly efficient industrial method of heterogeneous-catalytic conversion of natural gas remains relevant.

The task of the invention is to develop a high-performance method of processing natural gas and other gas mixtures with a predominant content of methane in the liquid at N.U. the mixture of hydrocarbons (C5-C8).

The inventive method is characterized by the following set of essential features.

A gas mixture of mainly methane and gas-oxidizer is passed at a temperature of 200-700°With primary and d is the pressure at the inlet of 1-50 atmospheres through a modified natural mineral shungite, containing from 90 to 95 wt.% the carbon component comprising from 20 to 90 wt.% nanocarbon forms, up to 70 wt.% which have opened channels show catalytic ability, or through the mentioned modified shungite as media included in an amount up to 2 wt.% metal socialization.

As the gas mixture with a predominant content of methane using natural gas or associated gas. As the gas-oxidant use oxygen or air.

A gas mixture of mainly methane and gas-oxidizer is passed through a modified shungite in continuous or pulsed mode.

As the metal catalyst, is introduced into a carrier-modified shungite, use heavy or transition metals or their oxides.

The preferred process temperature 300-350°C.

The set of essential features of the claimed method provides receive the following technical result:

- improve the performance of the method of processing natural gas for the following parameters: conversion WITH up to 40%, the selectivity for methane up to 35%, the specific activity of more than 2500, which exceeds the specifications of the prototype method;

- obtain the target product with a good yield and with almost no impurities. When i.e. monitoring) reference and the proposed method is achieved by dehydrogenation of methane from the formation of a mixture of branched and normal saturated hydrocarbons (C 5-C7) with a small admixture of alkenes and aromatic compounds (up to 5 wt.%) when the fullness of methane conversion in naphthas fraction up to 40 wt.%. In one cycle of the processing of natural gas output of hydrocarbons is, wt.%: ethane (C2H6) - no more than 2, propane (C3H8and isopropane - no more than 3, isomers of butane (C4H10) - not more than 5, mixture of isomers of pentane, hexane, heptane, nonane (C5H12With6H14C7H16C8H18) - 25-30, a mixture of alkenes (CnH2n) - not more than 5, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - not more than 5. Other products of the reaction are: unreacted methane (CH4), carbon monoxide (CO), hydrogen (H2), a mixture of alcohols methanol and ethanol (CH3HE, C2H5OH);

- reduce the cost of the target product by: (a) the use of cheaper catalyst manufactured from natural raw materials; (b) repeated use of the catalyst, which is not subject to ageing and degradation; (b) reduce energy intensity and (d) increasing the productivity of the process.

Distinguishing the essential features of the claimed method from the prototype method are the signs associated with the use of natural gas conversion catalyst - modificirovana what about the natural shungite as such or with the addition of heavy or transition metals or their compounds, and process conditions of the process in more mild conditions at a temperature of 200°and atmospheric pressure (the lower bound stated interval parameters).

The analysis of the prior art did not allow to find a solution that exactly matches the set of essential characteristics with declare that confirms the novelty of the method.

In the experiments described in: Grigorieva E.N., Rozhkova N.N. Shungite carbon behaviour in the modeling reactions of coal thermal decomposition // J. Appl. Chem. 2000. V.73, no. 4. P.600-605, found that powdered mineral shungite itself has some catalytic properties. This information does not affect the novelty of the claimed invention, because the catalytic effect is insignificant and the continuation of the experiments with unmodified stones hopeless from the point of view of getting the real work of the industrial catalyst.

Only the set of essential features of the proposed method allows to achieve the technical result. Despite the well-known attempts to use artificial nanocarbon (fulleroid) materials - processing products of fullerene soot - as catalysts, including processing of methane, all of them are limited to laboratory scale and have the disadvantages of negaranya is authorized by the reproducibility of the nanostructure catalysts during their own obtain and uncontrollability of nanotube growth catalyst during high-temperature reforming of natural gas. In addition, the high cost of the process closes currently the way to its industrial use. Therefore, there is the strong opinion of experts that nanotechnology in this area require further technological development and hardware design. The authors of the claimed invention, used is the only known natural mineral containing natural nanocarbon forms - shungite. The structure of the carbon content of the mineral described relatively recently: Zaidenberg A.Z., Rozhkova N.N., Kovalevsky, V.V. et al. Physical Chemical Model of Fullerene-like Shungite rocks // Mol. Mat. 1996. V.8. P.107. Natural resources of shungite is very large, and its price is relatively low. The mineral in its pure form is not suitable as a catalyst, as it contains natural impurities. Due to the fact that the removal of impurities requires processing of mineral oxidants and high temperature exposure, which can cause damage to the nanostructures, to date, focused work on getting nanocarbon material from shungite is unknown. Therefore, to predict the quality of the catalyst modified enriched nanoforum shungite was impossible. Also unexpected were the results of the developed technology the conversion of natural gas: in more mild conditions than in counterparts, achieved the best performance and you are the od of the target product.

Thus, the claimed method meets the condition of patentability "inventive step".

To confirm the conformity of the invention the condition of "industrial applicability" below are examples of its specific implementation.

Modified natural mineral shungite obtained by the developed by the inventors of the technology lies in the fact that shungite is treated consistently when heated with alkali, concentrated inorganic acid, and optionally also a strong oxidant, after processing each of the reagents formed intermediate product is washed with water until neutral pH and dried, and then subjected to final processing of gas-phase oxidant in a high temperature furnace at temperatures up to 1200°C. the Resulting modified shungite according to electron microscopy contains from 90 to 95 wt.% the carbon component comprising from 20 to 90 wt.% nanocarbon forms, up to 70 wt.% which have opened channels.

Introduction to modified shungite is a carrier of a metal catalyst was carried out as follows.

The Introduction Of Pd. Modified shungite was soaked in a 10 wt.% an aqueous solution of palladium nitrate Pd(NO3)2, was dried in air at a temperature of 100°and progulivali at a temperature of 950-1000° C. the Pd Content up to 2 wt.%.

Introduction Mo. Modified shungite was soaked in a 10 wt.% aqueous solution of paramolybdate ammonium (NH4)2Mo4, was dried in air at a temperature of 100°and progulivali at a temperature of 700-750°C. the Content of Mo, up to 2 wt.%.

The Introduction Of Ti. Modified shungite was soaked in a 10 wt.% aqueous solution of TiCl4, was dried in air at a temperature of 300°and progulivali at a temperature of 900-950°C. the Content of Ti in the form of TiO2- up to 2 wt.%.

Similarly implemented the introduction of other catalysts, such as Pt, V, and oxides of heavy and transition metals.

To conduct process gas mixtures with a predominant content of methane used the standard heterogeneous-catalytic reactor (GTR). When this catalyst was placed between two metal grids in GTR.

The authors of the claimed invention found that a modified natural mineral shungite has a great natural material specific surface area (200 to 1000 m2/g) and sorption properties with respect to pairs of hydrocarbons (primarily methane - 10-12 wt.% when N.U.), to hydrogen (up to 2-3 wt.% when N.U.), carbon oxide (II), oxygen - and nitrogen-containing compounds, and transition and heavy metals from their solutions in a wide interval for the Les of temperature and pressure. This suggested high efficiency modified shungite when used as a heterogeneous catalyst for natural gas processing.

When testing the modified shungite as a heterogeneous catalyst in the range of temperature values 200-700°C and pressures up to 30 ATM, the authors observed an effective dehydrogenation of methane from the formation of a mixture of branched and normal saturated hydrocarbons (C5-C8) with a small admixture of alkenes and aromatic compounds (up to 5 wt.%) when the fullness of methane conversion in basin-ligroin fraction up to 40 wt.%. Aging and/or degradation of the catalysts modified shungite with multiple quoting process was not observed. The catalytic effect is greatly enhanced by the introduction of modified shungite some heavy and transition metals (Ti, Zr, Al, Ru and the like) in the form of metals, oxides, salts in quantities (1-2 wt.%).

Example 1.

Taken heterogeneous catalytic reactor (GTR) of 70 cm3in it were placed 40 g of the catalyst - modified shungite. The composition of the modified shungite: carbon component - 95 wt.% (here and everywhere next % by weight of the total weight of the catalyst), nano-form - 90 wt.%, disclosed nanotubes - 70 wt.%. Used continuous input mode in GTR nature is underwater gas (containing 97 wt.% methane and gas-oxidizer oxygen and output of the synthesis product. The onset temperature of the process amounted to 400°C. a Primary inlet pressure in the reactor was 30 ATM.

The result is a mixture of hydrocarbons in the following quantities: ethane (C2H6) - 0.7 wt.%, propane (C3H8) - 1 wt.%, the isomers of butane (C4H10) - 1.5 wt.%, the mixture of isomers of pentane, hexane, heptane, nonane (C5H12With6H14C7H16C8H18) - 23 wt.%, a mixture of alkenes (CnH2n) to 0.8 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - 4 wt.%. Other products of the reaction are: unreacted methane (CH4), carbon monoxide (CO), hydrogen (H2), a mixture of alcohols methanol and ethanol (CH3HE, C2H5OH).

Example 2 (temperature variation).

The experiment was conducted similarly to example 1, but the temperature of the beginning of the process amounted to 350°C. the resulting mixture of hydrocarbons in the following quantities: (C2H6) to 0.9 wt.%, (C3H8) - 1.3 wt.%, (C4H10) - 1.5 wt.%, mixture of isomers (C5H12With6H14C7H16C8H18) - 18 wt.%, a mixture of alkenes (CnH2n) - 0.3 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene and 2.5 wt.%.

Example 3 (variation of temperature).

The experiment was conducted similarly to example 1, is, however, the onset temperature of the process amounted to 200° C. the resulting mixture of hydrocarbons mixture of isomers of pentane, hexane, heptane, nonane (C5H12With6H14C7H16C8H18) amounted to 17 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - 0.7 wt.%.

Example 4 (variation of temperature).

The experiment was conducted similarly to example 1, but the temperature of the beginning of the process amounted to 700°C. the resulting mixture of hydrocarbons mixture of isomers of pentane, hexane, heptane, nonane (C5H12With6H14C7H16C8H18) amounted to 26 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - 4.2 wt.%.

Example 5 (a variation of the primary pressure at the inlet of the reactor).

The experiment was conducted similarly to example 1, however, the primary pressure at the inlet to the beginning of the process amounted to 15 ATM. The result is a mixture of hydrocarbons in the following quantities: (C2H6) - 1.3 wt.%, (C3H8) - 1.7 wt.%, (C4H10) - 1.2 wt.%, mixture of isomers (C5H12With6H14C7H16C8H18) - 17 wt.%, a mixture of alkenes (CnH2n) - 0.3 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - 3 wt.%.

Example 6 (a variation of the primary pressure at the inlet of the reactor).

The experiment was conducted similarly to example 1, however, the primary pressure is at the entrance to the beginning of the process was 1 ATM. The resulting mixture of hydrocarbons mixture of isomers of pentane, hexane, heptane, nonane (C5H12With6H14C7H16C8H18) 17.6 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - 2.1 wt.%.

Example 7 (a variation of the primary pressure at the inlet of the reactor).

The experiment was conducted similarly to example 1, however, the primary pressure at the inlet to the beginning of the process amounted to 50 ATM. The resulting mixture of hydrocarbons mixture of isomers of pentane, hexane, heptane, nonane (C5H12With6H14C7H16C8H18) amounted to 30 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - 5.1 wt.%.

Example 8 (a variation of the composition of the oxidizing agent).

The experiment was conducted similarly to example 1, however, as the gas-oxidant instead of oxygen consumed air. The result is a mixture of hydrocarbons in the following quantities: (C2H6) - 0.7 wt.%, (C3H8) - 0.7 wt.%, (C4H10) to 0.9 wt.%, mixture of isomers (C5H12With6H14C7H16C8H18) - 16 wt.%, a mixture of alkenes (CnH2n) - 0.5 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene) - 1.5 wt.%.

Example 9 (a variation of the continuous - pulsed).

The experiment was conducted similarly to example 1,but in a pulsed mode (reset pressure in the reactor to 1 ATM 1 every 10 min). The result is a mixture of hydrocarbons in the following quantities: (C2H6) - 1.1 wt.%, (C3H8) - 3.1 wt.%, (C4H10) - 4 wt.%, mixture of isomers (C5H12With6H14C7H16C8H18) - 33 wt.%, a mixture of alkenes (CnH2n) - 2.9 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - 5 wt.%.

Mentioned pulse mode is used for desorption and removal of products of synthesis of alkanes C5-C8from the surface of the heterogeneous catalyst and prevents further oligomerization get alkanes.

Example 10 (variation of the catalyst composition).

The experiment was conducted similarly to example 1, but used a modified shungite with palladium - 0.1 wt.%. The result is a mixture of hydrocarbons in the following quantities: (C2H6) - 1.3 wt.%, (C3H8) - 2.6 wt.%, (C4H10) - 3.1 wt.%, mixture of isomers (C5H12With6H14C7H16C8H18) - 29 wt.%, a mixture of alkenes (CnH2n) of 4.1 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - 4.9 wt.%.

Example 11 (a variation of the catalyst composition).

The experiment was conducted similarly to example 1, but used a modified shungite with titanium oxide and 1.5 wt.%. The result is a mixture of hydrocarbons in the following the respective quantities: ethane (C 2H6) to 0.9 wt.%, propane (C3H8) - 1.5 wt.%, the isomers of butane (C4H10) - 1.9 wt.%, the mixture of isomers of pentane, hexane, heptane, nonane (C5H12With6H14C7H16C8H18) - 25 wt.%, a mixture of alkenes (CnH2n) to 0.9 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - 4.1 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene) - 4.2 wt.%.

Example 12 (a variation of the catalyst composition).

The experiment was conducted similarly to example 1, but used a modified shungite with molybdenum - 2 wt.%. The resulting mixture of hydrocarbons mixture of isomers of pentane, hexane, heptane, nonane (C5H12With6H14C7H16C8H18) amounted to 24 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - 4.9 wt.%.

Example 13 (a variation of the catalyst composition).

The experiment was conducted similarly to example 1, but used a modified shungite with platinum - 0.2 wt.%. The resulting mixture of hydrocarbons mixture of isomers of pentane, hexane, heptane, nonane (C5H12With6H14C7H16C8H18) amounted to 31 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - 3.7 wt.%.

Example 14 (a variation of the composition of the modified shungite)

Experience conducting is similar to example 1, but used the modified shungite following composition: carbon component is 90 wt.%, nanocarbon forms - 20 wt.%, disclosed nanotubes are practically absent. The resulting mixture of hydrocarbons mixture of isomers of pentane, hexane, heptane, nonane (C5H12With6H14C7H16C8H18) was 21 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - 4 wt.%.

Example 15 (a variation of the composition of the modified shungite)

The experiment was conducted similarly to example 1, but used a modified shungite following composition: carbon component is 90 wt.%, nanocarbon forms - 20 wt.%, disclosed nanotubes - 20 wt.%. The resulting mixture of hydrocarbons mixture of isomers of pentane, hexane, heptane, nonane (C5H12With6H14C7H16C8H18) amounted to 25 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - 4.1 wt.%.

Example 16 (a variation of the original gas mixture).

The experiment was conducted similarly to example 1, but used a synthesis gas containing 81% by weight carbon monoxide CO and 19 wt.% of hydrogen. The resulting mixture of hydrocarbons mixture of isomers of pentane, hexane, heptane, nonane (C5H12With6H14C7H16C8H18) amounted to 22 wt.%, mixture of aromatic Ugledar is. benzene, toluene, isomers of xylene - 4.1 wt.%.

Example 17 (a variation of the original gas mixture).

The experiment was conducted similarly to example 1, but used associated gas containing 91 wt.% methane and 9 wt.% a mixture of ethane, propane, isopropane, butane and isobutane. The resulting mixture of hydrocarbons mixture of isomers of pentane, hexane, heptane, nonane (C5H12With6H14C7H16C8H18) amounted to 27.3 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - 5.1 wt.%.

Example 18 (a variation of the original gas mixture)

The experiment was conducted similarly to example 1, but used the condensate. The resulting mixture of hydrocarbons mixture of isomers of pentane, hexane, heptane, nonane (C5H12With6H14C7H16C8H18) amounted to 33 wt.%, a mixture of aromatic hydrocarbons - benzene, toluene, isomers of xylene - 4.1 wt.%.

Experiments under the conditions described in examples 1, 6, 16, was held without rebooting GTR up to 100 times. Lowering of catalytic activity and the selectivity of the process was not observed.

Implementation of the claimed invention is not limited to the above examples.

The results given in examples 1-18, suggests that the implementation of the claimed invention results in comparison with the known method of the prototype to the improving the performance of the method of processing gases, mainly methane, namely:

achieving the conversion of methane to liquid hydrocarbons (C5H12With6H14With7H16With8H18- up to 35%;

the achievement of the specific activity (i.e. number of moles of methane CH4convertible to 1 g of catalyst) - more than 2,500;

to obtain the desired product in good yield and with almost no impurities;

the reduction process due to the use of cheaper reusable catalyst;

energy saving due to the milder conditions of the processing gas.

Moving beyond the specified ranges of parameter values reduces the efficiency of the process and leads to the impossibility of implementing the claimed invention on an industrial scale.

1. Method of heterogeneous-catalytic conversion of gas mixture mainly of methane, which consists in the fact that the gas mixture and the gas-oxidizer is passed at a temperature of 200-700°and pressure of 1-50 atmospheres through a modified natural mineral shungite containing from 90 to 95 wt.% the carbon component comprising from 20 to 90 wt.% nanocarbon forms, up to 70 wt.% which have open channels, and show catalytic ability, or through the mentioned modified shungite as media included in an amount up to 2 wt.% metal Katalizator is.

2. The method according to claim 1, characterized in that the gas mixture using natural gas or associated gas.

3. The method according to claim 1, characterized in that as the gas-oxidant use oxygen or air.

4. The method according to claim 1, characterized in that the said gas mixture and the gas-oxidizer is passed through a modified shungite in continuous or pulsed mode.

5. The method according to claim 1, characterized in that, as mentioned metal catalyst used heavy or transition metals or their oxides.

6. The method according to claim 1, wherein the nanocarbon forms in the carbon component of shungite include nanotubes, nanoarray, neolocality, nano-cones.



 

Same patents:

FIELD: crude oil treatment.

SUBSTANCE: invention relates to methods of treatment of crude oil before subsequent transportation, in particular to treatment of sulfur crude oils and gas condensates with high contents of hydrogen sulfide and mercaptans. Treatment of hydrogen sulfide-containing crude oil is carried out via multistep separation and blow-out with hydrocarbon gas either in low-pressure separation step or in additional desorption column at 25-80°C and pressure 0.1-0.5 MPa until degree of removal of hydrogen sulfide contained in crude achieves 55-90% followed by neutralization of remaining amounts of hydrogen sulfide by adding, at stirring, effective amounts of 20-40% water-alkali solution of sodium nitrite with pH at least 11 or 18-40% aqueous solution of sodium sulfite and sodium bisulfite at sulfite-to-bisulfite molar ratio 1:(0.3-0.9). In this case, sodium nitrite water-alkali solution is added on the basis of 0.9-2.0 mole (preferably 1-1.5 mole) nitrite and aqueous solution of sodium sulfite and bisulfite on the basis of 1-2 mole sulfite and bisulfite per 1 mole residual hydrogen sulfide. When treating hydrogen sulfide and mercaptan-containing crude, the latter is added with 0.9-2 mole (preferably 1-1.5 mole) nitrite per 1 mole residual hydrogen sulfide and light methyl- and ethylmercaptans. Alkali agent in above water-alkali solution of sodium nitrite is sodium hydroxide and/or water-soluble organic amine. Hydrocarbon gas used for the blow-up is preliminarily liberated from hydrogen sulfide separation gas from H2S-containing crude oil or low-sulfur petroleum gas, or natural gas preferably used on the basis of 2.5 to 10 m3/m3 oil.

EFFECT: increased efficiency of process due to elimination of pollution of commercial petroleum with nitrogen-organic compounds and use of accessible, inexpensive, and less toxic neutralizer, simultaneous neutralization of petroleum acids, reduced acidity and corrosiveness of treated commercial petroleum.

9 cl, 1 dwg, 1 tbl, 8 ex

FIELD: organic synthesis catalysts.

SUBSTANCE: invention relates to methods for preparing catalyst precursors and group VIII metal-based catalysts on carrier, and to a process of producing hydrocarbons from synthesis gas using catalyst of invention. Preparation of precursor of group VIII metal-based catalyst comprises: (i) imposing mechanical energy to mixture containing refractory oxide, combining catalyst precursor with water to form paste comprising at least 60 wt % of solids, wherein ratio of size of particles present in system in the end of stage (i) to that in the beginning of stage (i) ranges from 0.02 to 0.5; (ii) mixing above prepared paste with water to form suspension containing no more than 55% solids; (iii) formation and drying of suspension from stage (ii); and (iv) calcination. Described are also method of preparing group VIII metal-based catalyst using catalyst precursor involving reduction reaction and process for production of hydrocarbons by bringing carbon monoxide into contact with hydrogen are elevated temperature and pressure in presence of above-prepared catalyst.

EFFECT: increased catalytic activity and selectivity.

12 cl, 1 tbl, 3 ex

FIELD: separation of organic compounds.

SUBSTANCE: invention concerns adsorption isolation processes and can be used when isolating monomethyl-substituted paraffins from hydrocarbon mixtures. Gist of invention resides in that a method for adsorption isolation with simulated moving bed designed for isolation of monomethyl-substituted paraffin C8-C14 is realized by passing initial mixture through adsorbent bed at air/fuel ratio between 0.5 and 1.5, 30-120°C, and operation cycle time 20-60 min. Thereafter, adsorbed monomethyl-substituted paraffin is selectively isolated from adsorbent bed when in contact with desorbent. Initial mixture containing monomethyl-substituted paraffins further contains at least another acyclic nonlinear hydrocarbon with the same number of carbon atoms and less than 5% of normal C8-C14-paraffins. Adsorbent includes silicate.

EFFECT: increased selectivity of isolation.

10 cl

FIELD: petroleum processing and lubricants.

SUBSTANCE: lubricating oil fraction is preliminarily combined with low-boiling hydrocarbon solvent and stepwise extraction is then conducted at 40-55°C using dimethylsulfoxide as selective solvent.

EFFECT: increased degree of purification without using surfactants complicating and raising in price purification process, reduced consumption of solvent (by 30-40%) and power.

1 tbl, 4 ex

FIELD: petroleum processing.

SUBSTANCE: process, which is, in particular, suitable in production of raw materials for secondary processes via purification of petroleum residues with hydrocarbon solvents, is characterized by that, after purification of petroleum residues, organic solvent is regenerated by stripping solvent contained in purification products and in wax solution, freed from hydrogen sulfide, compressed and recycled into process. Compression of solvent is performed in flow compressor employing as working medium solvent vapors withdrawn from dewaxed solution evaporator.

EFFECT: reduced loss of solvent, reduced consumption of water steam, and improved quality of dewaxed product and wax.

3 cl, 1 dwg, 1 tbl, 4 ex

FIELD: oil production and transportation, particularly to prevent pipeline corrosion in and to protect environment.

SUBSTANCE: method involves mixing fine iron powder having particle dimensions of not more than 20 μm with well product, wherein the iron powder is added in amount of 16 g per 1 l of well product; stirring iron powder and well product for 15 min; holding the mixture for 12 hours; removing the resultant iron sulfide with the use of magnetic separator.

EFFECT: prevention of pipeline corrosion, increased oil product quality and improved ecological protection.

1 ex

FIELD: petroleum processing.

SUBSTANCE: invention, in particular, relates to purification of vacuum gas oils, mazuts, and/or dewaxed products used further as feedstock for hydrocracking and catalytic cracking as well as high-quality fuel oils and marine oils. Purification contemplates removal of polycyclic aromatic hydrocarbons, heteroatomic compounds, resins, asphaltenes, and heavy metal compounds. Process consists in liquid extraction of undesired components with two mutually immiscible solvents: polar N-methylpyrrolidone with 3-5% water at 40-60°C and nonpolar n-undecane or undecane fraction forming azeotropic mixtures with N-methylpyrrolidone having minimal boiling temperature (about 179°C). Weight ratio of nonpolar solvent to raw material is (0.4-0.5):1.

EFFECT: increased selectivity of process in reduced risk of thermooxidative and hydrolytic decomposition of N-methylpyrrolidone as well as corrosion of equipment.

1 dwg, 4 tbl, 4 ex

FIELD: petroleum processing and petrochemistry.

SUBSTANCE: invention, in particular, relates to removing at least some trace impurities from liquid hydrocarbon fuels and to a method for clearing gasoline hydrocarbon fuel. Invention especially concerns those impurities selected from inanes, naphthalenes, phenantrenes, pyrene, alkylbenzenes, and mixtures thereof. At least a part of liquid hydrocarbon fuel, which is gasoline, is brought into contact with decolorizing activated carbon according to method disclosed in the present application. Employment of resulting gasoline in spark-ignition engines or at least in one zone in engine intake system is also described.

EFFECT: reduced formation of deposits in engines.

18 cl, 1 dwg, 2 tbl, 2 ex

FIELD: crude oil treatment and petroleum processing.

SUBSTANCE: removal of hydrogen sulfide and mercaptans from crude oil and gas condensate is accomplished by directly heating oil well produce in hydrocyclone and treating released gases together with steam-gas mixture by hydrogen sulfide- and mercaptan-selective reagent: aqueous solution of 1-hydroxy-2[1,3-oxazetidin]-3-yl-ethane (C4H9O2N) followed by cooling at temperature not higher than 15°C and separation at pressure at least 1.3 excessive atm. Installation has stilling manifold, depulser, separators, hydrocyclone, condenser-cooler, gasoline separator, discharge pumps, buffer vessel, and tanks. Accumulation tank for cleaned product is provided with heated hydrocyclone having diminishing cone angle and steam-gas line exit connected to gasoline separator equipped with mass-exchange bulk attachment.

EFFECT: considerably improved quality of well produce and reduced loss of raw material.

2 cl, 3 dwg

FIELD: crude oil treatment.

SUBSTANCE: invention relates to removal of hydrogen sulfide and mercaptans from petroleum and gas condensate. Process is conducted through oxidation of impurities with air oxygen dissolved in petroleum under pressure up to 2.5 MPa at 20 to 70°C in presence of solution of ammonium salts of cobalt sulfophthalocyanines in 20-30% aqueous ammonia solution. Reagents are used in following amounts calculated per 1 mole hydrogen sulfide: 0.1-1.6 mole NH4OH, 0.05-0.1 g phthalocyanine catalyst, and 0.05-0.1 m3 air. More specifically, ammonium salts of cobalt sulfo-, disulfo-, tetrasulfo-, dichlorodisulfo-, and dichlorodioxydisulfophthalocyanine are used. Part of exhausted ammonia catalyst solution is separated from cleaned raw material and returned into process.

EFFECT: minimized consumption of reagents and power, and enabled carrying out the process directly under oil-field conditions.

10 cl, 1 dwg, 2 tbl, 3 ex

FIELD: polymer production.

SUBSTANCE: invention relates to processing of polyvinylchloride-based compositions for manufacturing film materials and simulated leather. Composition according to invention comprises polyvinylchloride, dioctyl phthalate stabilizer, and 4-(2,3-epoxypropoxy)-4'-alkyloxyazoxybenzene having general formula:

, wherein n=1-10.

EFFECT: increased resistance of material to light and heat effects, reduced toxicity, and simplified formula of composition.

2 tbl

FIELD: organic chemistry, medicine, oncology.

SUBSTANCE: invention relates to organic amine salts, amino acid salts and combrestatin A-4 phosphate amino acid ester salts. Invention describes compound of the general formula (I):

wherein one of substitute -OR1 or -OR represents -O-QH+ and another one represents hydroxyl or -O-QH+; Q represents (A) optionally substituted aliphatic organic amine comprising at least one nitrogen atom that in common with proton forms quaternary ammonium cation QH+; (B) amino acid comprising at least two nitrogen atoms wherein one of nitrogen atoms in common with proton forms quaternary ammonium cation QH+; (C) amino acid comprising one or some nitrogen atoms wherein one of nitrogen atoms in common with proton forms quaternary ammonium cation QH+ and wherein, except for, all carboxyl groups of amino acids are in ester form. Also, invention describes pharmaceutical compositions used in modulation of tumor or metastasis proliferation and growth of benign vascular proliferative disorders, using compound of the formula (I) and a method for synthesis of compound of the formula (I). Invention provides preparing new combrestatin A-4 salts showing useful physicochemical properties that enhance solubility of combrestatin A-4.

EFFECT: valuable medicinal properties of compounds and pharmaceutical compositions.

27 cl, 13 dwg, 5 ex

FIELD: organic chemistry, medicine, oncology.

SUBSTANCE: invention relates to organic amine salts, amino acid salts and combrestatin A-4 phosphate amino acid ester salts. Invention describes compound of the general formula (I):

wherein one of substitute -OR1 or -OR represents -O-QH+ and another one represents hydroxyl or -O-QH+; Q represents (A) optionally substituted aliphatic organic amine comprising at least one nitrogen atom that in common with proton forms quaternary ammonium cation QH+; (B) amino acid comprising at least two nitrogen atoms wherein one of nitrogen atoms in common with proton forms quaternary ammonium cation QH+; (C) amino acid comprising one or some nitrogen atoms wherein one of nitrogen atoms in common with proton forms quaternary ammonium cation QH+ and wherein, except for, all carboxyl groups of amino acids are in ester form. Also, invention describes pharmaceutical compositions used in modulation of tumor or metastasis proliferation and growth of benign vascular proliferative disorders, using compound of the formula (I) and a method for synthesis of compound of the formula (I). Invention provides preparing new combrestatin A-4 salts showing useful physicochemical properties that enhance solubility of combrestatin A-4.

EFFECT: valuable medicinal properties of compounds and pharmaceutical compositions.

27 cl, 13 dwg, 5 ex

FIELD: organic chemistry, medicine, oncology.

SUBSTANCE: invention relates to organic amine salts, amino acid salts and combrestatin A-4 phosphate amino acid ester salts. Invention describes compound of the general formula (I):

wherein one of substitute -OR1 or -OR represents -O-QH+ and another one represents hydroxyl or -O-QH+; Q represents (A) optionally substituted aliphatic organic amine comprising at least one nitrogen atom that in common with proton forms quaternary ammonium cation QH+; (B) amino acid comprising at least two nitrogen atoms wherein one of nitrogen atoms in common with proton forms quaternary ammonium cation QH+; (C) amino acid comprising one or some nitrogen atoms wherein one of nitrogen atoms in common with proton forms quaternary ammonium cation QH+ and wherein, except for, all carboxyl groups of amino acids are in ester form. Also, invention describes pharmaceutical compositions used in modulation of tumor or metastasis proliferation and growth of benign vascular proliferative disorders, using compound of the formula (I) and a method for synthesis of compound of the formula (I). Invention provides preparing new combrestatin A-4 salts showing useful physicochemical properties that enhance solubility of combrestatin A-4.

EFFECT: valuable medicinal properties of compounds and pharmaceutical compositions.

27 cl, 13 dwg, 5 ex

FIELD: organic chemistry, medicine, oncology.

SUBSTANCE: invention relates to organic amine salts, amino acid salts and combrestatin A-4 phosphate amino acid ester salts. Invention describes compound of the general formula (I):

wherein one of substitute -OR1 or -OR represents -O-QH+ and another one represents hydroxyl or -O-QH+; Q represents (A) optionally substituted aliphatic organic amine comprising at least one nitrogen atom that in common with proton forms quaternary ammonium cation QH+; (B) amino acid comprising at least two nitrogen atoms wherein one of nitrogen atoms in common with proton forms quaternary ammonium cation QH+; (C) amino acid comprising one or some nitrogen atoms wherein one of nitrogen atoms in common with proton forms quaternary ammonium cation QH+ and wherein, except for, all carboxyl groups of amino acids are in ester form. Also, invention describes pharmaceutical compositions used in modulation of tumor or metastasis proliferation and growth of benign vascular proliferative disorders, using compound of the formula (I) and a method for synthesis of compound of the formula (I). Invention provides preparing new combrestatin A-4 salts showing useful physicochemical properties that enhance solubility of combrestatin A-4.

EFFECT: valuable medicinal properties of compounds and pharmaceutical compositions.

27 cl, 13 dwg, 5 ex

FIELD: organic chemistry, medicine, oncology.

SUBSTANCE: invention relates to organic amine salts, amino acid salts and combrestatin A-4 phosphate amino acid ester salts. Invention describes compound of the general formula (I):

wherein one of substitute -OR1 or -OR represents -O-QH+ and another one represents hydroxyl or -O-QH+; Q represents (A) optionally substituted aliphatic organic amine comprising at least one nitrogen atom that in common with proton forms quaternary ammonium cation QH+; (B) amino acid comprising at least two nitrogen atoms wherein one of nitrogen atoms in common with proton forms quaternary ammonium cation QH+; (C) amino acid comprising one or some nitrogen atoms wherein one of nitrogen atoms in common with proton forms quaternary ammonium cation QH+ and wherein, except for, all carboxyl groups of amino acids are in ester form. Also, invention describes pharmaceutical compositions used in modulation of tumor or metastasis proliferation and growth of benign vascular proliferative disorders, using compound of the formula (I) and a method for synthesis of compound of the formula (I). Invention provides preparing new combrestatin A-4 salts showing useful physicochemical properties that enhance solubility of combrestatin A-4.

EFFECT: valuable medicinal properties of compounds and pharmaceutical compositions.

27 cl, 13 dwg, 5 ex

FIELD: organic chemistry, medicine, oncology.

SUBSTANCE: invention relates to organic amine salts, amino acid salts and combrestatin A-4 phosphate amino acid ester salts. Invention describes compound of the general formula (I):

wherein one of substitute -OR1 or -OR represents -O-QH+ and another one represents hydroxyl or -O-QH+; Q represents (A) optionally substituted aliphatic organic amine comprising at least one nitrogen atom that in common with proton forms quaternary ammonium cation QH+; (B) amino acid comprising at least two nitrogen atoms wherein one of nitrogen atoms in common with proton forms quaternary ammonium cation QH+; (C) amino acid comprising one or some nitrogen atoms wherein one of nitrogen atoms in common with proton forms quaternary ammonium cation QH+ and wherein, except for, all carboxyl groups of amino acids are in ester form. Also, invention describes pharmaceutical compositions used in modulation of tumor or metastasis proliferation and growth of benign vascular proliferative disorders, using compound of the formula (I) and a method for synthesis of compound of the formula (I). Invention provides preparing new combrestatin A-4 salts showing useful physicochemical properties that enhance solubility of combrestatin A-4.

EFFECT: valuable medicinal properties of compounds and pharmaceutical compositions.

27 cl, 13 dwg, 5 ex

FIELD: organic chemistry, chemical technology, medicine.

SUBSTANCE: invention relates to the improved method for synthesis of 1,3-substituted indenes that are intermediate compounds used in synthesis of aryl-condensed azapolycyclic compounds used in treatment of neurological and psychological disorders. Method for synthesis of 1,3-substituted indenes of the general formula (I) given in the invention description wherein R1 represents electron-accepting group chosen from the group consisting of cyano-group, alkoxycarbonyl, alkylcarbonyl, aryl, nitro-group, trifluoromethyl and sulfonyl; R2 and R3 are chosen independently from hydrogen atom, (C1-C5)-alkyl, (C1-C5)-alkoxy-group, trifluoromethyl, halogen atom, sulfonylalkyl, alkylamino-group, amide, ester, arylalkyl, heteroalkyl and arylalkoxy-group; or R2 and R3 in common with carbon atoms to which they are bound form monocyclic or bicyclic ring; each R4 represents independently (C1-C6)-alkyl, or two groups of R4 form in common (C2-C3)-alkylene bridge involves the following steps: (a) interaction in the absence of solvent between compound of the formula (II) given in the invention description wherein X is chosen from the group consisting of chlorine, bromine and iodine atoms, and R1, R2 and R3 have above given values with monohydric or dihydric alcohol in the presence of sulfuric acid, and (b) treatment of the reaction product with base and water for neutralization o sulfuric acid residue. As a rule, compound of the formula (II) is synthesized by (a) interaction of compound of the formula (III) given in the invention description wherein R1, R2, R3 and X have above given values with 3-ethocyacrylate in the presence of catalyst and inert water-soluble organic solvent, and (b) complete removal of solvent after termination of indicated reaction. Method provides preparing 1,3-substituted indenes with high yield.

EFFECT: improved method of synthesis.

13 cl, 3 sch, 1 ex

FIELD: organic chemistry, chemical technology, medicine.

SUBSTANCE: invention relates to the improved method for synthesis of 1,3-substituted indenes that are intermediate compounds used in synthesis of aryl-condensed azapolycyclic compounds used in treatment of neurological and psychological disorders. Method for synthesis of 1,3-substituted indenes of the general formula (I) given in the invention description wherein R1 represents electron-accepting group chosen from the group consisting of cyano-group, alkoxycarbonyl, alkylcarbonyl, aryl, nitro-group, trifluoromethyl and sulfonyl; R2 and R3 are chosen independently from hydrogen atom, (C1-C5)-alkyl, (C1-C5)-alkoxy-group, trifluoromethyl, halogen atom, sulfonylalkyl, alkylamino-group, amide, ester, arylalkyl, heteroalkyl and arylalkoxy-group; or R2 and R3 in common with carbon atoms to which they are bound form monocyclic or bicyclic ring; each R4 represents independently (C1-C6)-alkyl, or two groups of R4 form in common (C2-C3)-alkylene bridge involves the following steps: (a) interaction in the absence of solvent between compound of the formula (II) given in the invention description wherein X is chosen from the group consisting of chlorine, bromine and iodine atoms, and R1, R2 and R3 have above given values with monohydric or dihydric alcohol in the presence of sulfuric acid, and (b) treatment of the reaction product with base and water for neutralization o sulfuric acid residue. As a rule, compound of the formula (II) is synthesized by (a) interaction of compound of the formula (III) given in the invention description wherein R1, R2, R3 and X have above given values with 3-ethocyacrylate in the presence of catalyst and inert water-soluble organic solvent, and (b) complete removal of solvent after termination of indicated reaction. Method provides preparing 1,3-substituted indenes with high yield.

EFFECT: improved method of synthesis.

13 cl, 3 sch, 1 ex

FIELD: chemical industry, chemical technology.

SUBSTANCE: invention relates to synthesis of 4-(2,3-epoxypropoxy)-4'-propyloxyazobenzene eliciting properties of light-thermostabilizing agent for polyvinyl chloride.

EFFECT: valuable properties of compound.

2 tbl, 1 ex

FIELD: hydrogenation-dehydrogenation catalysts.

SUBSTANCE: catalyst composition intended for hydrogen processing contains component of non-precious metal of group VIII, two components of group VIB metals, and 1 to 30% of combustible binder including at least 50 wt % carbon.

EFFECT: achieved preparation of high-strength catalyst easily controllable during a process.

17 cl

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