Zeolite catalyst, method to manufacture thereof and method to convert straight-run gasoline to high-octane number component

FIELD: CHEMISTRY.

SUBSTANCE: zeolite catalyst for process of conversion of straight-run gasoline to high-octane number component is described. The said catalyst contains high-silica zeolite with SiO2/Al2O3=60 and residual content of Na2О of 0.02 wt.% maximum, metal-modified, Pt, Ni, Zn or Fe metals being in nanopowder form. Content of the said metals in the catalyst is 1.5 wt.% maximum. Method to manufacture zeolite catalyst for conversion of straight-run gasoline to high-octane number component is described. The said method implies metal modification of zeolite, Pt, Ni, Zn or Fe metals being added to zeolite as nanopowders, produced by electric explosion of metal wire in argon, by dry pebble mixing in air at room temperature. Method to convert straight-run gasoline using the said catalyst is also described.

EFFECT: increase in catalyst activity and gasoline octane number, accompanied by increase in yield.

4 cl, 3 tbl, 4 ex

 

The invention relates to the refining and petrochemical industries, in particular to a method for producing catalysts for the conversion of straight-run gasoline fractions of crude oil into high-octane component of gasoline.

Known zeolite-containing catalyst and method for producing it high-octane gasoline and aromatic hydrocarbons (RF patent No. 2087191, 1997). The catalyst includes zeolite group Pancasila, oxide of zinc, oxide of rare earth element, a binder component and further comprises an oxide of boron and fluorine, and as a rare earth element or two or more oxides selected from the group of lanthanides: lanthanum oxide, cerium oxide, neodymium oxide, praseodymium oxide, and has the following content, wt.%: zeolite 20,0-70,0; zinc oxide 1.0 to 4.0; the oxides of rare earth elements 0,1-2,0; boron oxide is 0.1 to 3.0; a fluoride of 0.1 to 3.0; a binder component is rest. The method of transformation of aliphatic hydrocarbon, C2-C12in high-octane gasoline and aromatic hydrocarbons by contact of them with the catalyst at 280-550°C, a pressure of 0.5 to 3.0 MPa and space velocity of the raw material of 0.5 to 3.0 HR-1.

Known zeolite-containing catalyst for the conversion of aliphatic hydrocarbons, C2-C12in high octane gasoline which is enriched in aromatic hydrocarbons (RF patent No. 2092240, 1997. The catalyst contains a zeolite group pentasil with silicate module SiO2/Al2O3=20-80 mol/mol and a residual content of Na2O of 0.1-0.4 wt.%, a binder component, zinc and a mixture of oxides of rare earth elements in the following ratio, wt.%: zeolite 25,0-50,0; zinc 1,0-3,0; the sum of the oxides of rare earth elements 0,1-2,0, representing a mixture of the following composition, wt.%: CeO240,0-55,0); the amount of La2About3Pr2O3Nd2O360,0-45,0; a binder component is rest. The method of transformation of aliphatic hydrocarbon, C2-C12in high-octane gasoline and aromatic hydrocarbons by contact of them with the catalyst at 480-550°C, a pressure of 0.5 to 3.0 MPa and space velocity of the raw material of 0.5 to 3.0 HR-1.

Known zeolite-containing catalyst and method for the conversion of aliphatic hydrocarbons, C2-C12in a high-octane component of gasoline or a concentrate of aromatic hydrocarbons (RF patent No. 2100075, 1997). The catalyst contains a zeolite group pentasil with silicate module SiO2/Al2O3=20-80 mol/mol and a residual content of Na2O not more than 0.2 wt.%, a binder component, the oxides of zinc and rare earth elements as promoters, it is additionally contains P2O5when using as the oxides redkozemel the data elements of two or more of the following: CeO 2La2O3Pr2O3Nd2O3in the following, wt.%: zeolite 50,0-75,0; ZnO 0,5-3,0; the sum of the oxides of rare earth elements from 0.5 to 3.0; P2O50.5 to 2.0; a binder component is rest. The method of transformation of aliphatic hydrocarbon, C2-C12in a high-octane component of motor gasoline with an octane rating of at least 76 points by the motor method or a concentrate of aromatic hydrocarbons is carried out by contact of the catalyst with the feedstock at a temperature 280-550°C, a pressure of 0.2 to 2.0 MPa and space velocity of the raw material of 0.5 to 5.0 h-1.

Known methods for producing motor fuels from gas condensate (RF patents №№2008323, 1994 and 2030446, 1995). Straight-run gasoline fraction in contact with 300-480°and 0.2-4.0 MPa with a zeolite-containing catalyst. The products obtained fractionary with gaseous and liquid fraction, the liquid fraction rectificatum emitting high-octane and residual fractions. Straight-run residual fraction or its mixture with gaseous products of the probe is subjected to pyrolysis. The products obtained fractionary with the release of pyrolysis condensate fraction and pyrogas, followed by mixing the pyrogas with straight-run gasoline fraction and their joint contact with the catalyst. The pyrolysis condensate fraction compounding with liquid the food probe and expose their joint rectification with a target allocation of gasoline and residual fractions. As the catalyst systems prepared on the basis of zeolites with structures of ZSM-5 or ZSM-11, including modified items I, II, III, V, VI and VIII groups of the Periodic system of elements.

A known method of producing motor fuel from crude oil (RF patent No. 2176661, 2001). Carry out hydrocracking of oil and release of the products of hydrocracking gasoline and middle distillates. Catalytic conversion is subjected to straight-run gasoline and at least the hard part of the gasoline produced in the hydrocracking using a catalyst containing zeolite group Pancasila and hydrogenating/dehydrating component, in the conditions of formation of aromatic hydrocarbons from paraffins and naphthenes.

Known methods for producing high-octane gasoline fractions and aromatic hydrocarbons with two or more reaction zones (application for invention№№97101099, 1999; 93013854, 1997; RF patent №2039790, 1995). Hydrocarbons, wikipaedia in the temperature range of the boiling point of gasoline is subjected to serial communication in the reaction zone with a catalyst based on zeolite ZSM-5 or ZSM-11, including modified items I, II, III, IV, and VIII groups. At the same time in each subsequent zone is subjected to contacting a light gasoline fraction of the previous zone, and heavy gasoline fractions zones is mixed with the liquid product is chami contact of the last zone. Stage contacting is carried out at 300-480°With (better 320-460° (C) and a pressure of 0.2 to 4.0 MPa (preferably 0.5 to 4.0 MPa).

The disadvantages of these methods of obtaining zeolite catalysts is their complex composition and the presence of harmful effluents in their manufacture, and the need to use in their synthesis of fluorine (RF patent No. 2087191, 1997), high residual content of sodium oxide and low mass fraction of the active portion of the catalyst, which significantly reduces its performance on the target product, an irreversible reduction in the activity of zinc-containing catalysts in the ablation of zinc in the conditions of high temperature reaction and catalyst regeneration (RF patent No. 2092240, 1997), the need to apply phosphorus oxide, which settle on the acid centers of the zeolite, first, reduces the amount of strong acid sites of the zeolite, and, secondly, it reduces the effective radius of the pores of the zeolite, creating additional steric hindrance to the raw material components (RF patent No. 2100075, 1997), as well as their high cost, due to the use of expensive oxides of rare earth elements.

The disadvantages of these methods for the production of motor fuels is a complex multistage process flowchart (RF patents №№2008323, 1994 and 2030446, 1995), the need for preliminary hydrocracking used for the processing of raw materials(patent RF №2176661, 2001), the use of two or more reaction zones (application for invention№№97101099, 1999; 93013854, 1997; RF patent №2039790, 1995).

Closest to the claimed catalyst is a zeolite-containing catalyst and method for the conversion of aliphatic hydrocarbons in the concentrate of aromatic hydrocarbons or high-octane component of gasoline (RF patent No. 2221643, 2004). Zeolite-containing catalyst contains zeolite group pentasil with silicate module SiO2/Al2O3=55-102 mol/mol and a residual content of sodium oxide of 0.02-0.07 wt.%, the oxides of zinc, tin and lanthanum as elements of the structure of the zeolite, and as a promoter oxide of chromium, at the following content, wt.%: zeolite 65,0-80,0; ZnO 0,0-4,0; Zr2About30,0-0,8; SnO20,0-2,5; Cr2About30,0-5,0; Na2O 0,02-0,07, the binder component is rest. There is also described a method of transformation of aliphatic hydrocarbons in the concentrate of aromatic hydrocarbons or high-octane component of gasoline (options) by passing vapors of straight-run gasoline fractions of oil through a bed of the zeolite catalyst at a temperature of 300-380°C, atmospheric pressure and the load of the catalyst raw materials 2 h-1. The yield of the final product is not less than 67%.

The main disadvantages of this zeolite-containing catalyst is its complex status is in and the associated multi-technological scheme of production, the cooking time, as well as the need for the use of the oxide of rare earth elements (lanthanum oxide). This zeolite-containing catalyst, process for its production and method of use we have chosen as a prototype. Output, octane number and group composition of gasolines obtained by the method prototype, shown in table 1.

The proposed zeolite catalyst, process for its production and a way of turning straight-run gasoline fraction of petroleum with its use eliminates these drawbacks.

The technical result concerning the method of obtaining a zeolite catalyst is achieved by the fact that Pt/HZSM-5, Ni/HZSM-5 and Zn/HZSM-5 or Fe/HZSM-5 catalysts obtained by dry mechanical mixing on the air zeolite HZSM-5 with a molar ratio of SiO2/Al2O3=60 (M=60) and APC Pt, Ni, Zn or Fe obtained by electrical explosion of wire metals in argon. The concentration of APCS metal in the zeolite catalyst is 1.5 wt.%. The catalytic activity of the prepared systems under the same process conditions higher than that of catalysts prepared "traditional" methods of modification of zeolite HZSM-5 - method of ion exchange from aqueous solutions of the corresponding salts or the introduction of relevant elements at the stage of hydrothermal synthesis of the zeolite.

Technical re the query result on the way, based on the proposed use of the zeolite catalyst for the conversion of straight-run gasoline fractions of crude oil into high-octane gasoline components, is achieved by passing vapors of straight-run gasoline fractions of crude oil (raw material) through the catalyst bed heated to a temperature of 300-400°s, when the load of the catalyst raw materials 2 h-1and atmospheric pressure.

The advantages offered by the zeolite catalyst are simplified method modification (mechanical mixing), lack of sewage and opportunities with it high-octane component of gasoline with an octane rating of at least 80 points from a straight-run gasoline fraction of petroleum.

Further, the invention is illustrated with specific examples of its implementation.

Example 1. To 4.0 g decationizing zeolite H-ZSM-5 (M=60) added 0.06 g APCS Pt (1.5 wt%), obtained by the method of electrical explosion of wire metal in argon. The resulting mixture was mixed in a vibratory mill for 0.5 h in air at room temperature. Then the catalyst was pressed into tablets, cut up and taken away for research fraction of 0.5-1.0 mm

Catalytic testing of the samples is carried out in flow-through installation at the reaction temperature of 300-400°C, space velocity straight-run gasoline fraction 2 h-1

Analysis of transformation products straight-run gasoline fraction oil is conducted every 60 min of operation of the catalyst by gas chromatography, the octane number of gasoline is determined by calculation on the basis of chromatographic data.

Output group composition and octane number of the gasoline obtained are shown in table 2.

Example 2. In the same way as in example 1, but instead of APC Pt add APCS Ni (1,5% by weight of zeolite).

Output group composition and octane number of the gasoline obtained are shown in table 2.

Example 3. In the same way as in example 1, but instead of APC Pt add APCS Zn (1.5% of the weight of the zeolite).

Output group composition and octane number of the gasoline obtained are shown in table 3.

Example 4. In the same way as in example 1, but instead of APC Pt add APC Fe (1.5% of the weight of the zeolite).

Output group composition and octane number of the gasoline obtained are shown in table 3.

As can be seen from the data tables, the proposed catalyst and its production method differs from the prototype higher activity and allows you to increase the octane number of gasoline is while increasing its output in the process of turning straight-run gasoline fraction of petroleum.

Table 1

Comparative characteristics of the activity of zeolite catalysts (prototype)
IndicatorsPrototype
Example 1Example 2
Process temperature, °300340360380300340360380
The output of gasoline, %8779757088757367
The product yield, wt.%
Alkanes With3-C412,54,82,81,69,68,66,96,1
Alkenes With3-C41,10,60,30,30,60,80,80,6
N-alkanes With5+9,16,86,2of 5.48,96,76,0the 5.7
ISO-alkanes With5+39,033,9 29,328,536,534,933,333,2
Alkenes With5+5,24,2the 3.83,23,02,82,82,8
Cycloalkanes9,28,07,87,18,08,27,47,7
Arena23,941,749,853,9the 33.438,042,843,9
Octane number7883868781838484

td align="center"> 88
Table 2

Comparative characteristics of high activity zeolite modified APCS Pt and Ni (example 1 and 2)
IndicatorsIn example 1 and 2
Pt/HZSM-5Ni/HZSM-5
Process temperature, °300340360380300340360380
The output of gasoline, %91857690837669
The product yield, wt.%
Alkanes With3-C411,511,010,87,69,5the 9.77,67,5
Alkenes With3-C41,00,80,60,40,60,71,60,4
N-alkanes With5+4,2a 3.93,02,76,95,14,13,0
ISO-alkanes With5+39,037,325,423,741,031,932,327,3
Alkenes With5+3,23,31,70,92,01,91,70,9
Cycloalkanes2,22,01,82,12,11,01,41,7
Arena38,941,756,662,6of 37.949,754,3 59,2
Octane number8790919686909193

Table 3

Comparative characteristics of high activity zeolite modified APCS Zn and Fe (example 3 and 4)
IndicatorsFor example 3 and 4
Zn/HZSM-5Fe/HZSM-5
Process temperature, °300340360380300340360380
The output of gasoline, %8681786979696361
The product yield, wt.%
Alkanes With3-C411,111,27,14,56,66,85,8the 3.8
Alkenes With3-C41,10,60,50,40,20,21,31,1
N-alkanes With5+ 9,4the 5.75,05,16,96,47,56,6
ISO-alkanes With5+29,327,128,423,530,9of 31.433,130,4
Alkenes With5+5,22,22,01,41,71,62,82,2
Cycloalkanes1,20,80,70,96,56,73,23,0
Arena42,752,3of 60.564,4to 47.246,946,352,9
Octane number8891939491929294

1. The zeolite catalyst process for the conversion of straight-run gasoline fractions of crude oil into high-octane component of gasoline, incorporating high-silica zeolite with a molar ratio of SiO2/Al2O3=60 and the residual content of Na2O not more than 0.02 wt.%, modified metals, wherein the metals Pt, Ni, Zn or Fe are shown the in the catalyst in the form of nano-sized powders, the content of these metals in the catalyst is not more than 1.5 wt.%.

2. The method of preparation of the zeolite catalyst according to claim 1 for the conversion of straight-run gasoline fractions of crude oil into high-octane component of gasoline, including the modification of zeolite metals, characterized in that the modifying metals Pt, Ni, Zn or Fe is introduced into the zeolite in the form of nanosized metal powders obtained by electrical explosion of wire metal in an argon atmosphere by dry mechanical mixing in a ball mill at room temperature.

3. A way of turning straight-run gasoline fractions of crude oil into high-octane component of gasoline in the presence of a zeolite catalyst, characterized in that the use of the catalyst according to claim 1.



 

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FIELD: petrochemical processes.

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