Method of producing high octane gasoline fractions

 

(57) Abstract:

Usage: in the petrochemical industry, in particular in the processing of hydrocarbon raw materials. The inventive method involves contacting the hydrocarbon ( boiling point up to 200 to 220°C ) in an environment of hydrogen containing gas with a catalyst containing zeolites, including zeolite with structure of ZSM-5 or ZSM-11, the metals of the second, third, fourth, eighth group, and/or compounds of metals of the first - fourth group in the presence of carbon monoxide (2+and/or carbon dioxide (4+). The process is carried out at 280 460°C., a pressure of 0.3 to 10.0 MPa, mass flow rate of feed of 0.2 to 10.0 wt. h/wt. h per hour space velocity of hydrogen containing gas 1000 22100 about. PM/about.h. per hour, a molar ratio of hydrogen and the mixture monoxide and carbon dioxide, equal to 1 to 20, and the molar ratio of carbon monoxide to the dioxide, equal to 0.02 1000. When using raw materials containing paraffins and naphthenes, the process is carried out at 350 to 440°C., a pressure of 1 to 10 MPa, feedstock containing olefins, at 300 and 400°C., a pressure of 0.5 to 6 MPa. 7 C.p. f-crystals, 6 PL.

The invention relates to a catalytic process for the production of unleaded high-octane gasoline fractions from the hydrocarbon is adnie faction, wikipaedia at the temperature of boiling gasoline (up to 200-220aboutC) and gaseous registereda faction.

Known methods for producing gasoline fractions and their high-octane components of hydrocarbons in the environment of the hydrogen-containing gas, for example [1-3] According to the methods of conversion of various hydrocarbons WITH2-C12carried out in the temperature intervals of the reaction 200-700aboutWith the speed of feed of 0.1-400 h-1when the molar ratio of N2/Plevo - Dorogi to 20 on the catalysts containing zeolites of type ZSM, including modified by various elements. The main disadvantages of these methods or relatively low yields or low octane gasolines produced.

The closest in technical essence is a way to hydroprene hydrocarbons [4] According to the selected prototype high-octane gasoline fraction obtained by contacting the hydrocarbons WITH1-C12at a temperature of 250-700aboutC, a pressure of 0.1-10 MPa, the space velocity of the raw material of 0.5-10 h-1and the molar ratio of N2/hydrocarbons 50 with a catalyst based on zeolites, including ZSM. The catalyst may contain IU torida 1-80, metal is 0.1-30 wt. The main disadvantages of the prototype are relatively low-octane gasoline fractions obtained.

The invention consists in contacting the hydrocarbon feedstock with zeolite catalyst at elevated temperature and pressure in the environment of the hydrogen-containing gas in the presence of carbon monoxide II and/or carbon monoxide IV (CO, CO2). The reaction products separated from gaseous and liquid (gasoline) fractions. Stage contacting is carried out in temperature ranges of reactions 280-460aboutC, a pressure of 0.3 to 10 MPa, mass flow rate of feed of hydrocarbons from 0.2 to 10 h-1, volumetric feed rate of the hydrogen-containing gas 1000-22100 h-1and the molar ratios of H2/CO+CO21-20 and CO/CO2=-0-1000.

As raw materials is possible using liquid hydrocarbon fractions, wikipaedia in the temperature range of the boiling point of gasoline (up to 200-220aboutS), and/or gaseous registergui fractions. Optimal processing of paraffin-naphthene raw material (a process called "Sinar") are the reaction temperature 350-440aboutC and a pressure of 4-10 MPa, and for processing registertimer (C2-C5) raw materials (protonirovannogo or modified elements I, II, III, VI and VIII groups of the zeolite, 0-70% of oxides of elements I, II, III, VI groups and 0-30% of a binder. As zeolite using zeolites with structure of ZSM-5 or ZSM-11 General formula aNa2O bAl2O3the bot dSiO2(where enOmone or more oxides of elements I-VIII groups, and the coefficients a, b, c and d depend on the method of preparation of the zeolite, or zeolite type Y or mordenite or beta; zeolites (after synthesis) can be modified by items I, II, III, VI and VIII groups; zeolites, including modified, prepared by the known methods. The composition of the catalyst of oxides of elements I, II, III, VI groups described General formula (aCuO+bZnO+cAl2O3+dCr2O3+eW2O5), where a=0-60, b=24-67, C=0-10, d=0-33, e=0-1 wt.

The main advantages of the proposed method are higher octane number gasolines produced.

The main distinctive feature of the invention, the implementation stage contacting of the feedstock with the catalyst in the presence of carbon monoxide II and/or carbon monoxide IV.

Industrial applicability of the invention is illustrated as follows: example 1 prototype examples 2-6 equivalents of the prototype and is shown for comparison, examples 7-33 the proposed method.

P IS SUB>5+0,1) is subjected to contacting with the catalyst in the environment of hydrogen at a molar ratio of N2/CH=3, a temperature of 300aboutWith and the weight of the feed rate of the raw material 1 h-1. The catalyst contains, by weight, 80. zeolite H-ZSM-5 and 20% AlF3. In the contact formed 75% of hydrocarbon gases and 25% gasoline5+containing 52% of aromatic hydrocarbons.

P R I m m e R 2. Straight-run gasoline fraction 40-150aboutWith octane PTS= 62 MM and the composition is shown in table. 3, is subjected to contacting with the catalyst 1 (composition shown in table. 2) in the environment of hydrogen at the reaction temperature Tp=380aboutC, pressure P=8.0 MPa, the mass feed rate of the raw material g=1.5 h-1and flow rate of gas (hydrogen) W=2300 h-1. The reaction products separated from the allocation of 17.5 wt. hydrocarbon gases and 82.5% gasoline PTS=69,3 MM and composition is shown in table. 3.

P R I m e R 3. Analogous to example 2. Model hydrocarbon fraction 68-146aboutWith the estimated octane OCHp=46 MM and the composition is shown in table. 4, is subjected to contacting with the catalyst 1 (composition shown in table. 2) at Tp= 380aboutC, P=8.0 MPa, g=1.4 CH-1and W=3000 h-1. Prva, are given in table. 4.

P R I m e R s 4-6. Analogous to example 2. Hydrocarbons hexene-1 is subjected to contacting with the catalyst in the environment of hydrogen at the reaction temperature Tp, the pressure P, the mass feed rate of the raw material g and the volumetric rate of gas supply W. Products contact share with gaseous and liquid (gasoline) fractions. The process conditions are given in table. 1, the compositions of the catalysts in table. 2, the compositions obtained gasoline fractions in the table. 5.

Examples 7-33 the proposed method.

P R I m e R 7. Straight-run gasoline fraction 40-150aboutWith octane PTS=62 MM and the composition is shown in table. 3, is subjected to contacting with the catalyst 1 in the presence of CO and CO2in the environment of the hydrogen-containing gas composition, vol. H267,1; 30,0; CO20,3; CH4+N22,6. The process of contacting is carried out at a reaction temperature Tp=380aboutC, pressure P=8.0 MPa, the mass feed rate of the raw material g=1.5 h-1, space velocity gas W=2300 h-1and the molar ratio of N2/CO+CO22.2 and CO/CO2100. Hydrocarbon reaction products separated with the separation of 19.4 wt. hydrocarbon gases and 80.6% gasoline fraction with a logical example 7. In example 9 the molar ratio of N2/CO+CO220, and the ratio of CO/CO226. The process conditions are given in table. 1, the compositions of the catalysts in table. 2. outputs, composition and octane number of the gasoline obtained in table. 3.

P R I m e R 10. Similar to example 7. The contacting with the catalyst 4 (composition shown in table. 2) in the environment of hydrogen gas (H250,3% about. WITH 48,9; CO20,05; N2-0,75) is subjected to model hydrocarbon fraction WITH6-C9with the estimated octane OCHp=-8 and composition is shown in table. 3, the contacting is carried out at Tp= 420aboutC, P= 4.0 MPa, g=1.4 CH-1W=1540 h-1N2/CO+CO21,0 and CO/CO21000. Hydrocarbon reaction products separated with the separation of 30.5 wt. hydrocarbon gases and 69.5% gasoline-OCHp= 38 and composition is shown in table. 3.

P R I m e R 11. Similar to example 7. The contacting with the catalyst 1 (composition shown in table. 2) in the environment of hydrogen gas (H267,1 about. WITH 30,0; CO20,3; CH4+N22,6) subjecting a hydrocarbon fraction 63-125aboutWith octane OCHp= 48 MM and the composition is shown in table. 4. The contacting is carried out at Tp=380

P R I m e R 12-14. Similar to example 7. Use raw materials of example 11 (composition shown in table. 4); the process conditions are given in table. 1; the compositions of the catalysts in table. 2; and outputs the compositions obtained gasoline in the table. 4. The octane number of the gasoline produced in example 12 PTS 78 MM.

P R I m e R s 15-16. Similar to example 7. Hydrocarbons (n-hexane in example 15; n-octane (example 16) is subjected to contacting with the catalyst at the reaction temperature Tr of the pressure P, the mass feed rate of the raw material g, the volume rate of gas flow W, the molar ratio of N2/CO+CO21,8. The reaction products separated with separation of hydrocarbon gas and gasoline fractions of the composition given in table. 4. Hydrogen gas has the following composition, about. H262,8; 35,7; N21,5. The process conditions are given in table. 1, the catalyst composition in the table. 2.

P R I m e R 17. Similar to example 7. Hydrocarbons hexene-1, is subjected to contacting with the catalyst 1 (composition shown in table. 2) in the hydrogen-containing gas composition, vol. H271,3; 27,1; CO20,1; N21,5. Contacts provocatory the reaction products separated with the separation of 26.4 wt. hydrocarbon gases and 73,6% gasoline-PTS-79 MM and the composition is shown in table. 5.

P R I m e R s 18-26. Similar to example 7. As raw materials use of hexene-1. In example 22 molar ratio of N2/CO+CO21,3 and CO/CO20,02; for example 23 molar ratio of N2/CO+CO211.6 and CO/CO22,2; examples 24-25 molar ratio of N2/CO+CO22.7 and CO/CO2500; example 26 molar ratio of N2/CO+CO22,8 (content in gas CO2=0). The process conditions are given in table. 1; the compositions of the catalysts in table. 2; and outputs the compositions obtained gasoline in the table. 5. The octane number of the gasoline produced in example 21 PTS 62 MM.

P R I m e R s 27-28. Similar to example 7. Hydrocarbons consisting of 27.5 wt.h. fraction of n-paraffins (C6-50 wt. WITH7-35% WITH8-15% PTSp=10 MM) and 105,5 wt.h. registertimer gas (C2H43.8 wt. WITH3H617,8%3H80,2; N278,2% ) is subjected to contacting with the catalyst 9 in the environment of the hydrogen-containing gas composition, vol. H223,4; CO22,6; N274,0. The contacting is carried out at a reaction temperature Tr of the pressure P, the mass feed rate of the hydrocarbon raw material g, the AI is shared with the release of hydrocarbon gases and gasoline fractions. The process conditions are given in table. 1, the catalyst composition in the table. 2, the composition and the estimated octane number gasoline fraction in the table. 6.

P R I m e R s 29-33. Similar to example 7. Propane-propylene fraction (1: 4 wt.) subjected to contacting with the catalyst N 10 (composition shown in table. 2) in the hydrogen-containing gas. While the reaction gas has the following General composition, wt. WITH35,3; C3=21,1; N213,4; 14,8; CO214,7; N230,7. The contacting is carried out at a reaction temperature Tr of the pressure P, the mass feed rate of the hydrocarbon g, volumetric feed rate of the strip W, and a molar ratio of N2/CO+CO27,8 and CO/CO21,6. The process conditions, the yields of hydrocarbon products are shown in table. 1, the compositions of the catalysts in table. 2, the composition and the estimated octane number of the gasoline obtained in table. 6.

1. METHOD of producing high OCTANE GASOLINE FRACTIONS from wikipaedia 200 220oWith hydrocarbons by contacting in an environment of hydrogen containing gas at elevated temperature and pressure with a catalyst containing zeolites, including zeolite with structure of ZSM-5 or ZSM-11, metals, II, III, VI and VIII groups and/or compounds of the metal is and carbon IV.

2. The method according to p. 1, characterized in that the contacting is carried out at a temperature of 280 460oC, a pressure of 0.3 to 10.0 MPa, the weight of the feed rate of raw materials 0,2 10,0 r-1, volumetric feed rate of the hydrogen-containing gas 1000 22100 r-1, a molar ratio of N2/CO + CO21oC 20 and the molar ratio of CO/CO20,02oC 1000.

3. The method according to p. 1, characterized in that the use of a catalyst containing a zeolite modified with elements I, II, III, VI and VIII groups.

4. The method according to p. 1, characterized in that the use of raw materials, mainly containing paraffins and naphthenes, the contacting is carried out at a temperature of 350 440oC, pressure of 1.0 to 10.0 MPa.

5. The method according to p. 1, characterized in that when using a raw material containing olefins, mainly WITH2WITH5the contacting is carried out at a temperature of 300 400oC, a pressure of 0.5 to 6.0 MPa.

6. The method according to p. 1, characterized in that the use of a catalyst containing a zeolite of type V

7. The method according to p. 1, characterized in that the use of a catalyst containing a mordenite type zeolite.

8. The method according to p. 1, characterized in that the use of a catalyst containing a zeolite type of bet

 

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12 cl, 3 tbl, 22 ex

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FIELD: CHEMISTRY.

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4 cl, 3 tbl, 4 ex

FIELD: chemistry.

SUBSTANCE: invention describes zeolite-containing catalyst for transformation of aliphatic hydrocarbons C2-C12 to a mix of aromatic hydrocarbons or high-octane gasoline component containing zeolite ZSM-5 with silicate module SiO2/Al2O3=60-80 mol/mol and 0.02-0.05 wt % of residual sodium oxide content, zeolite structural element, promoter and binding component, with zirconium or zirconium and nickel oxides as zeolite structural component, and zinc oxide as promoter, at the following component ratio (wt %): zeolite 65.00-80.00; ZrO2 1.59-4.00; NiO 0-1.00; ZnO 0-5.00; Na2O 0.02-0.05, the rest being binding component. Also, a method for obtaining zeolite-containing catalyst is described, which involves mixing reagents, hydrothermal synthesis, flushing, drying and calcinations of sediment. The reaction mix of water solutions of aluminum, zirconium and nickel salts, sodium hydroxide, silicagel and/or aqueous silicate acid, inoculating zeolite crystals with ZSM-5 structure in Na or H-form, and structure-former, such as n-butanol, is placed in an autoclave, where hydrothermal synthesis is performed at 160-190°C for 10-20 hours with continuous stirring; the hydrothermal synthesis over, Na-form pulp of the zeolite is filtered; the obtained sediment is flushed with domestic water and transferred to salt ion exchange by processing by water ammonium chloride solution with heating and stirring of the pulp; the pulp obtained from salt ion exchange is filtered and flushed with demineralised water with residual sodium oxide content of 0.02-0.05 wt % on the basis of dried and calcinated product; flushed sediment of ammonium zeolite form proceeds to zinc promoter introduction and preparation of catalyst mass by mixing of ammonium zeolite form modified by zinc and active aluminum hydroxide; obtained catalyst mass is extruded and granulated; the granules are dried at 100-110°C and calcinated at 550-650°C; calcinated granules of zeolite-containing catalyst are sorted, ready fraction of zeolite-containing catalyst is separated, while the granule fraction under 2.5 mm is milled into homogenous powder and returned to the stage of catalyst mass preparation. The invention also describes method of transformation of aliphatic hydrocarbons to high-octane gasoline component or a mix of aromatic hydrocarbons (variants), involving heating and passing raw material (gasoline oil fraction direct sublimation vapours or gas mix of saturated C2-C4 hydrocarbons) through stationary layer of the aforesaid catalyst.

EFFECT: reduced number of components and synthesis stages of zeolite-containing catalyst; increased transformation degree of raw material; improved quality and yield of target products with the said catalyst.

4 cl, 8 tbl, 12 ex

FIELD: chemistry.

SUBSTANCE: invention refers to production method of high-octane gasoline fractions and/or aromatic hydrocarbons C6-C10 as follows, hydrocarbon materials is heated, evaporated and overheated to process temperature, thereafter providing its contact at temperature 320-480°C and excess pressure with periodically recyclable catalyst containing zeolite of composition ZSM-5 or ZSM-11. Then it is cooled. Contact products are partially condensed, separated into gaseous and liquid fractions by separation. Liquid products of separation are supplied as power primarily to the first distillation column for separation of hydrocarbon gases and liquid stable fraction. The latter is supplied to the second distillation column for separation of high-octane gasoline fraction, or aromatic hydrocarbon fraction, and heavy charge fraction. Gaseous fraction resulted from separation of contact products is supplied to the first distillation column, specifically to intermediate section between infeed and external reflux inlet. External reflux is liquid distillate of the first distillation column.

EFFECT: reduction of power inputs, i.e. quantities of heat and cooling agent, required for reaction products separation.

5 cl, 2 ex

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