A method of producing motor fuels

 

(57) Abstract:

Usage: petrochemistry. Essence: catalytic cracking of petroleum fractions is carried out in the presence of a catalyst consisting of 5-20% of zeolite Y with a molar ratio of silica : alumina equal to 4.5 to 9.5 and 80-95 wt. %, and aluminosilicate framework and having the following chemical composition, wt.%: aluminum oxide 5,5-9,5, oxides of rare earth elements 0,5-3,0, platinum is 0.0001 to 0.01, the iron oxide of 0.01-0.4, iron oxide of 0.01-0.4, calcium oxide is 0.01-0.5, the magnesium oxide of 0.001 to 0.5, the sodium oxide is 0.01-0.5, the silicon oxide rest. The method allows to increase the output of gasoline to increase the octane number of gasoline and reduce emissions of sulfur oxides in the regeneration of the catalyst in the environment. table 2.

The invention relates to the production of motor fuels and can be used in the process of catalytic cracking in the petroleum industry.

The known method for the production of motor fuels by cracking petroleum fractions using aluminosilicate zeolite catalyst in a ball and microspheric forms. In ball form, the catalyst contains 10-12 wt.% zeolite Y has a chemical composition, wt.%:

Alumina - 9-10

Hydroxy is anyh fractions over zeolite catalysts. Ed. by S. N. Hadjiev. M., Chemistry. 1982).

In microspherical form the catalyst contains 16-18 wt.% zeolite Y and has the following chemical composition, wt.%:

Alumina - 10-12

The oxides of rare earth elements - 2,5-3,0

Sodium oxide is 0.2 - 0.6

The silicon oxide - Rest

There is also known a method of cracking of oil fractions in the presence of an aluminosilicate zeolite catalysts with addition of trace platinum is 0.0001-0.1 wt. % (U.S. patent N 4429053, class B 01 J 29/12; French Patent N 2500326, class B 01 J 29/12; Yandiev L. A. Zakarin N. A. The cracking catalysts and zeolites. Proceedings of the Groznii, M., TSNIITENEFTEHIM, 1984, No. 38, S. 76-80).

Closest to the proposed method to the technical essence and the achieved result is a method of producing motor fuels by cracking petroleum fractions in the presence of platinocyanide rare earth aluminosilicate catalyst with a platinum content 0,00001-0,002% (Patent FR 2407745, 1979). The zeolite treated metal salt (II-VIII gr. is 12-60%; the catalyst also contains perhaps 75% clay, 20 to 50% of three-hydrate-Al2O3and inorganic binder type oxide.

The disadvantage of this method of obtaining motor tadaka the present invention is to increase the yield of gasoline fraction by increasing the activity and selectivity of the applied platinocyanide rare earth aluminosilicate catalyst.

The problem is solved by the proposed method for the production of motor fuels by catalytic cracking of oil fractions in the presence of platinocyanide rare earth aluminosilicate catalyst, which uses a catalyst consisting of 5-20 wt.% zeolite Y with a molar ratio of silica:alumina equal to 4.5 to 9.5, and 80-95 wt.% aluminosilicate framework and having a chemical composition, wt.%:

Alumina - 5,5-9,5

The oxides of rare earth elements - 0,5-3,0

Platinum is 0.0001 to 0.01

Iron oxide - 0,01-0,4

Calcium oxide is 0.01-0.5 to

Magnesium oxide is 0.001 to 0.5

The sodium oxide - 0,01-0,5

The silicon oxide - Rest

Process for the production of motor fuels by cracking petroleum fractions is as follows: spherical catalysts for the cracking of vacuum gas oil is carried out at a temperature of 450-480oC, flow rate of feed of 1.0-2.5 h-1the ratio of catalyst circulation 1,5-2,5 kg/kg; microspherical catalyst cracking is carried out at 470-510oC, flow rate of the raw material of 4.8 h-1the ratio of circulation 6.9 kg/kg

The catalyst is prepared by the following method.

Aqueous solutions of aluminum sulfate acidified with sulfuric th glass) concentration of NaOH 1.4 to 1.8 chequ./m3and suspension of zeolite NaY, containing 30-110 kg/m3zeolite are mixed in the mixer with the formation of the aluminosilicate zeolite-containing Hydrosol, which is then coagulated with 5-20oC and pH 7.5-8.5 in the hydrogel pellet form in a layer of mineral oil. Next, the hydrogel can be syneresis when 35-60oC for 6-24 hours Later hydrogel treated with an aqueous solution of nitrate or ammonium sulfate concentration of 5-20 kg/m3when 35-60oC for 12-36 h and an aqueous solution of nitrates of rare-earth elements concentrations of 1-5 kg/m3(based on the oxides of rare earth elements) within 24-36 h, or their mixture, washed with condensate water containing iron cations from 0.01 to 0.4 kg/m3, of calcium from 0.01 to 0.5 kg/m3magnesium 0,001-0,5 kg/m3(calculated as metal oxides) when 35-60oC for 8-24 h, washed with condensate water at 35-60oC for 8-24 h, dried at 110-190oC and calcined at 650-750oC for 12-24 h in a current of steam-air mixture.

Platinum is introduced into the catalyst by the addition of hexachloroplatinic acid, H2PtCl66H2O, the solution of aluminum sulfate in the amount is 0.0002-0.04 kg/m3(calculated as platinum) or in the number 0,0006-0,085 kg/m3 is some form hydrogel beads after washing is subjected to dispersion in water at 20 to 60oC, spray-dried at the temperature of inlet flue gas amounts to 400-650oC and output 160-190oC and calcination in a fluidized bed at 600-750oC for 12-24 h in a current of steam-air mixture.

Catalysts are also obtained by sieve separation of catalyst in ball form after the stage of drying and/or calcination with a sampling fraction of balls of diameter less than 2 mm and subsequent grinding to a fraction of 20-140 microns.

Below are examples of the preparation of the catalyst and method of producing motor fuels by cracking petroleum fractions in the presence of this catalyst.

Example 1. An aqueous solution of aluminum sulfate containing 20 kg/m3Al2O3and 70 kg/m3H2SO4, an aqueous solution of sodium silicate (liquid glass) concentration of NaOH 1.6 chequ./m3and suspension of zeolite containing 80 kg/m3NaY with a molar ratio of silica: alumina equal to 4.5, and hexachloroplatinic acid concentration 0,0008 kg/m3(calculated as platinum), are mixed in the mixer with the formation of a Hydrosol, coagulated in 5oC and a pH of 8.3 in the hydrogel pellet form in a layer of mineral oil. Then the hydrogel treated with an aqueous solution Sul the x element concentration of 1.5 kg/m3( based on the oxides of rare earth elements - ORSA) if 50oC for 36 h, washed with condensate water containing iron cations 0.01 kg/m3the cations of calcium 0.001 kg/m3the cations of magnesium 0.001 kg/m3when 50oC for 24 h, dried at 150oC and calcined at 750oC for 12 h in a current of steam-air mixture.

The resulting ball catalyst contains 10 wt.% zeolite has a composition, wt.%:

Alumina - 8,5

The oxides of rare earth elements - 2,5

Platinum - 0,0001

Iron oxide - 0,01

Calcium oxide is 0.01

Magnesium oxide - 0,001

The sodium oxide - 0,2

The silicon oxide - Rest

Example 2. An aqueous solution of aluminum sulfate containing 25 kg/m3Al2O3and 80 kg/m3H2SO4, an aqueous solution of sodium silicate (liquid glass) concentration of NaOH 1.8 chequ. /m3and suspension of zeolite containing 30 kg/m3NaY with a molar ratio of silica: alumina, 9.5, and hexachloroplatinic acid at concentrations of 0.015 kg/m3(calculated as platinum), are mixed in the mixer with the formation of a Hydrosol, coagulated in 5oC and pH 8.5 in the hydrogel pellet form in a layer of mineral oil. Then the hydrogel with a solution of nitrate of rare earth elements concentration of 5 kg/m3(based on the oxides of rare earth elements - ORSA) at the 35oC for 24 h, washed with condensate water containing iron cations 0.4 kg/m3the cations of calcium 0.5 kg/m3the cations of magnesium 0.5 kg/m3when 35oC for 24 h, dried at 110oC and calcined at 750oC for 12 h in a current of steam-air mixture.

The resulting ball catalyst contains 20 wt.% zeolite has a composition, wt.%:

Alumina - 9,5

The oxides of rare earth elements - 3,0

Platinum - 0,01

Iron oxide - 0,4

Calcium oxide is 0.5

Magnesium oxide is 0.5

The sodium oxide - 0,5

The silicon oxide - Rest

Example 3. An aqueous solution of aluminum sulfate containing 15 kg/m3Al2O3and 50 kg/m3H2SO4, an aqueous solution of sodium silicate (liquid glass) concentration of NaOH (1.4 chequ./m3and suspension of zeolite containing 110 kg/m3NaY with a molar ratio of silica: alumina equal to 6.2, and hexachloroplatinic acid concentration of 0.085 kg/m3(calculated as platinum), are mixed in the mixer with the formation of a Hydrosol, coagulated at 20oC and pH 7.5 in the hydrogel pellet form in a layer of mineral oil. Then the hydrogel by abrabam nitrates of rare-earth elements concentration of 1 kg/m3(based on the oxides of rare earth elements - ORSA) at 60oC for 36 h, washed with condensate water containing iron cations 0.1 kg/m3the cations of calcium 0.15 kg/m3the cations of magnesium 0.01 kg/m3at 60oC for 24 h, dried at 150oC and calcined at 750oC for 12 h in a current of steam-air mixture.

The resulting ball catalyst containing 5 wt.% zeolite has a composition, wt.%:

Alumina - 5,5

The oxides of rare earth elements - 0,5

Platinum - 0,004

Iron oxide - 0,1

Calcium oxide - 0,15

Magnesium oxide - 0,1

Sodium oxide is 0.01

The silicon oxide - Rest

Example 4. An aqueous solution of aluminum sulfate containing 20 kg/m3Al2O3and 70 kg/m3H2SO4, an aqueous solution of sodium silicate (liquid glass) concentration of NaOH 1.6 chequ./m3and suspension of zeolite containing 80 kg/m3NaY with a molar ratio of silica: alumina, 5.8, and hexachloroplatinic acid concentration is 0.0002 kg/m3(calculated as platinum), are mixed in the mixer with the formation of a Hydrosol, coagulated with 10oC and a pH of 8.3 in the hydrogel pellet form in a layer of mineral oil. Then the hydrogel by operatora nitrates of rare-earth elements concentration of 1.5 kg/m3(based on the oxides of rare earth elements - ORSA) if 50oC for 36 h, washed with condensate water containing iron cations 0.02 kg/m3the cations of calcium 0.02 kg/m3the cations of magnesium 0.001 kg/m3when 50oC for 24 h, dried at 150oC and calcined at 750oC for 12 h in a current of steam-air mixture.

The resulting ball catalyst contains 10 wt.% zeolite has a composition, wt.%:

Alumina - 8,5

The oxides of rare earth elements - 1,5

Platinum - 0,0001

Iron oxide - 0,2

Calcium oxide - 0,2

Magnesium oxide - 0,001

The sodium oxide - 0,15

The silicon oxide - Rest

Example 5. An aqueous solution of aluminum sulfate containing 20 kg/m3Al2O3and 0.04 kg/m3hexachloroplatinic acid (calculated as platinum) and 70 kg/m3H2SO4, an aqueous solution of sodium silicate (liquid glass) concentration of NaOH 1.6 chequ./m3and suspension of zeolite containing 80 kg/m3NaY with a molar ratio of silica:alumina, 5.8, are mixed in the mixer with the formation of a Hydrosol, coagulated with 10oC and a pH of 8.3 in the hydrogel pellet form in a layer of mineral oil. Then the hydrogel process vodno rare earth element concentration of 1.5 kg/m3(based on the oxides of rare earth elements - ORSA) if 50oC for 36 h, washed with condensate water containing iron cations 0.01 kg/cm3, calcium cations, 0.01 kg/m3the cations of magnesium 0.001 kg/m3when 50oC for 24 h, washed with condensate water at 50oC for 24 h, dried at 150oC and calcined at 750oC for 12 h in a current of steam-air mixture.

The resulting ball catalyst contains 12 wt.% zeolite has a composition, wt.%:

Alumina - 8,5

The oxides of rare earth elements - 1,5

Platinum - 0,01

Iron oxide - 0,01

Calcium oxide is 0.01

Magnesium oxide - 0,001

The sodium oxide - 0,2

The silicon oxide - Rest

Example 6. The catalyst is prepared analogously to example 5. Next, after washing the beads of hydrogel is subjected to dispersion in water at 50oC, spray-dried at the temperature of inlet flue gas 650oC and exit of flue gases 190oC and calcination in a fluidized bed at 750oC for 12 h in a current of steam-air mixture.

The resulting catalyst has a composition as in example 5.

Example 7. The catalyst is prepared analogously to example 5. Next, after washing the beads of hydrogel to be the C and outlet flue gas 160oC and calcination in a fluidized bed at 600oC for 24 h in a current of steam-air mixture.

The resulting catalyst has a composition as in example 5.

Example 8. The catalyst is prepared analogously to example 5. Next, after washing the beads of hydrogel is subjected to dispersion in water at 60oC, spray-dried at the temperature of inlet flue gas 500oC and exit of flue gases 175oC and calcination in a fluidized bed at 750oC for 24 h in a current of steam-air mixture.

The resulting catalyst has a composition as in example 5.

Example 9. The catalyst is prepared analogously to example 5. After calcination of the catalyst, it is subjected to sitonomy division and the fraction of balls of diameter less than 2 mm is subjected to grinding to obtain microspherical catalyst.

The resulting catalyst has a composition as in example 5.

Example 10. The catalyst obtained according to example 4 is used in the process of cracking of vacuum gasoil West Siberian oil. The process is carried out at pilot plant with a moving bed of the catalyst at the reaction temperature cracking 450oC, flow rate of feed of 1.0 h-1and the frequency of circulation of the catalyst is about gasoil West Siberian oil. The process is carried out at pilot plant with a moving bed of the catalyst at the reaction temperature cracking 480oC, space velocity of the raw materials 2.5 h-1and ratio of catalyst circulation 2.5 kg/kg

Example 12. Catalysts obtained in example 6, is used in the process of cracking of vacuum gasoil West Siberian oil. The process is carried out at pilot plant with a "boiling" layer of the catalyst at the reaction temperature cracking 470oC, space velocity of the raw material 4,0 h-1and ratio of catalyst circulation 6,0 kg/kg

Example 13. Catalysts obtained in example 6, is used in the process of cracking of vacuum gasoil West Siberian oil. The process is carried out at pilot plant with a "boiling" layer of the catalyst at the reaction temperature cracking 510oC, space velocity of the raw material 8,0 h-1and ratio of catalyst circulation 9,0 kg/kg

The obtained catalysts before laboratory tests are treated with 100% steam at 750oC within 6 hours of the Test ball catalysts carried out according OST 38.01176-79 at a temperature of 460oC and space velocity of the feedstock 1.5 h-1ü at 20oC 862 kg/m3the initial boiling point 203oC, the temperature of the end of the boil 360oC). Resulting catalysts have according OST 38.01161-78 at 480oC and the weight of the feed rate of the raw material 7,0 h-1. The results of laboratory tests are presented in table 1.

Ball catalysts obtained in examples 1 to 5, used in the process of cracking of vacuum gas oil from Western Siberian oil (density of 916 kg/m3the initial boiling point 512oC, the sulfur content of 1.6 wt.%). The process carried out at pilot plant with a moving bed of catalyst at a temperature of 460oC, space velocity of the feedstock 1.5 h-1the ratio of catalyst circulation 2 kg/kg

Resulting catalysts obtained in examples 6-9, used in the process of cracking of vacuum gasoil West Siberian oil. The process carried out at pilot plant with a "boiling" layer of the catalyst at a temperature of 480oC, the mass feed rate of the raw material 5 h-1the ratio of catalyst circulation 7 kg/kg

The results of pilot testing of ball and microspherical catalyst are presented in table 2.

Method for the production of motor fuels by Catalytica is utilizator, characterized in that the use of a catalyst consisting of 5 to 20 wt.% zeolite Y with a molar ratio of silica : alumina equal to 4.5 to 9.5 and 80 to 95 wt.% aluminosilicate framework and having a chemical composition, wt.%:

Alumina - 5,5 - 9,5

The oxides of rare earth elements - 0,5 - 3,0

Platinum is 0.0001 to 0.01

Iron oxide - 0,01 - 0,4

Calcium oxide is 0.01 - 0.5 to

Magnesium oxide is 0.001 to 0.5

The sodium oxide - 0,01 - 0,5

The silicon oxide - Rest

 

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14 cl, 1 ex

FIELD: chemistry.

SUBSTANCE: method includes contact of oil factions with catalyst, which contains hydride of embedding type of metal, having reaction surface, with obtaining mixture catalyst-oil fractions; supply of radio-frequency (RF) or microwave energy, at least, to one from catalyst and mixture catalyst-oil fractions; formation of single-atom hydrogen on reaction surface of hydride of embedding type of metal; and interaction of oil fractions with single-atom hydrogen. In other version method includes: contact of oil fractions with catalyst, containing hydride of embedding type of metal, which has reaction surface, with obtaining mixture catalyst-oil fractions; where hydride of metal of embedding type is obtained by introduction of hydrogen into metal alloy, selected from group consisting of 1) A1-xMxT5-y-zByCz, where x=0,0-1.0; y=0.0-2.5; z=0.0-0.5; A=Mm (mishmetal); T=Ni; M= at least one from La, Pr or Ce; B=Co; C= at least one from Mn, Al or Cr; 2) A2-xMxT14-yCyDzB, where x=0.0-2.0; y=0.0-14; z=0.0-3.0; A=Nd; T=Fe; M= at least one from La, Pr or Ce; B=boron; C=Co; D= at least one from Cr, Ni or Mn; 3) A2-xMxT1-yBy, where x=0.0-0.5; y=0.0-0.5; A=Mg; T= at least one from Ni or Cu; M=La; B= at least one from Fe or Co; and 4) their combinations; and supply of microwave or RF energy to, at least, one from catalyst and mixture catalyst-oil fractions. In third version method includes: contact of oil fraction with catalyst, containing hydride of embedding type of metal, which has reaction surface, forming single-atom hydrogen; and interaction of oil fractions with single-atom hydrogen; where hydride of metal of embedding type is obtained by introduction of hydrogen into metal alloy, selected from group consisting of 1) A1-xT5-y-zByCz, where x=0.0-1.0; y=0.0-2.5; z=0.0-0.5; A=Mm (mishmetal); T=Ni; M= at least one from La, Pr or Ce; B=Co; C= at least one from Mn, Al or Cr; 2) A2-xMxT14-yCyDzB, where x=0.0-2.0; y=0.0-14; z=0.0-3.0; A=Nd; T=Fe; M= at least one from La, Pr or Ce; B=boron; C=Co; D= at least one from Cr, Ni or Mn; 3) A2-xMxT1-yBy with x=0.0-0.5; y=0.0-0.5; A=Mg; T= at least one from Ni or Cu; M=La; B= at least one from Fe or Co; and 4) their combinations.

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31 cl, 8 ex, 10 tbl, 13 dwg

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