CN101130473A - Method and apparatus for steam dealkylation in a plant for the catalytic reforming of hydrocarbons - Google Patents
Method and apparatus for steam dealkylation in a plant for the catalytic reforming of hydrocarbons Download PDFInfo
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- CN101130473A CN101130473A CNA2007101426209A CN200710142620A CN101130473A CN 101130473 A CN101130473 A CN 101130473A CN A2007101426209 A CNA2007101426209 A CN A2007101426209A CN 200710142620 A CN200710142620 A CN 200710142620A CN 101130473 A CN101130473 A CN 101130473A
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- fraction
- steam dealkylation
- dealkylation
- hydrogen
- benzene
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts
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Abstract
The present invention describes a method for treating fractions (C6+ fractions) composed of hydrocarbon containing six carbon atoms; the fraction is formed in a device for catalytic reforming hydrocarbon-containing feeding, as well as an apparatus for applying the method. After hydrogenation, feeding the C6+ fractions for steam dealkylation, so as to generate usable product benzene and hydrogen.
Description
Technical field
The present invention relates to be used to handle main fraction (C by hydrocarbon composition with at least 6 carbon atoms
6+Fraction) method, this fraction are to form in the device that is used for the catalytic reforming hydrocarbonaceous feed, and the equipment that is used to implement this method.
Background technology
In the device that is used for the catalytic reforming hydrocarbonaceous feed, particularly process the heavier petroleum naphtha that for example in crude distillation, forms.
The heavier petroleum naphtha that for example forms in crude distillation contains different paraffin and positive paraffin especially, mainly has the naphthenic hydrocarbon and the aromatic hydrocarbons of 6 to 12 carbon atoms, and wherein the aromatic hydrocarbons part also can be considerably less and be depended on feed material.According to prior art, at first under the situation that consumes hydrogen and generation hydrogen sulfide, heavier petroleum naphtha is implemented desulfurization, send in the catforming process as feed material subsequently.In catalytic reforming, main paraffin and the naphthenic hydrocarbon that exists in the aromatic hydrocarbons that transforms under having the situation of catalyzer wherein produces hydrogen and light hydro carbons as by product.Isolate these by products from the reaction product of catalytic reforming, thereby form main fraction and main fraction (C by hydrocarbon composition with at least 6 carbon atoms by hydrogen and hydrocarbon composition with maximum 5 carbon atoms
6+Fraction).This C
6+Fraction contains aromatic hydrocarbons as can the economic product, particularly benzene that uses, and it is as the initial substance of synthetic many plastics, and is used to improve the antiknock value of gasoline.
In order to obtain C
6+Fraction can the economic product, particularly benzene that uses, and form maximum as far as possible productive rate, adopt following method according to prior art.Utilize liquid-liquid extraction by C
6+Fraction is isolated straight chain hydrocarbon, and continues to use as so-called raffinate, and this raffinate for example can be sent back in the feed material of catalytic reforming.C by straight chain hydrocarbon release
6+Fraction mainly contains the aromatic hydrocarbons with 6 to 8 carbon atoms now, and is separated into main fraction (mainly being benzene and toluene) and main fraction (mainly being dimethylbenzene) by the hydrocarbon composition with 8 carbon atoms by the hydrocarbon composition with 6 or 7 carbon atoms.Should mainly send into the method that is used for obtaining p-Xylol as feed material by the fraction of hydrocarbon composition with 8 carbon atoms.By mainly isolating benzene, then this fraction is sent in the process of hydrogen dealkylation as charging by the fraction of hydrocarbon composition with 6 or 7 carbon atoms.
For example WO 2005/071045 has described this type of and has been used for the method for hydrogen dealkylation.Exist under the situation of catalyzer in 400 to 650 ℃ temperature and 20 crust to the pressure of 40 crust hydro carbons to be contacted with hydrogen, wherein hydrogen exists with 3 to 6 times of molar excess of hydro carbons.Under these conditions, take off alkyl, thereby form benzene and various alkane (for example methane or ethane) from each alkylating aromatic hydrocarbons (for example toluene or dimethylbenzene) branch.
The consumption of hydrogen has negative impact according to prior art with the economy of the method that obtains benzene for these during the hydrogen dealkylation of hydro carbons.
Therefore, the objective of the invention is to develop selection at a kind of economy of prior art.
Summary of the invention
This purpose is to pass through C according to the present invention aspect method
6+Fraction is implemented steam dealkylation and is realized, wherein except such as two kinds of spendable product material benzene of main generation and the hydrogen reaction product of carbon monoxide and carbonic acid gas.
Basic thought of the present invention is by means of steam dealkylation alkylating aromatic hydrocarbons to be implemented dealkylation to produce benzene.Steam dealkylation only needs water vapor with low cost as feed material, and also produces valuable by product hydrogen except desired valuable product benzene.
Embodiment
The C that is used for steam dealkylation
6+Fraction mainly contains
A) have the aromatic hydrocarbons of 6 to 10 carbon atoms,
B) have the cyclic paraffins (naphthenic hydrocarbon) of 5 to 10 carbon atoms,
C) have the different paraffin and the positive paraffin of 5 to 10 carbon atoms,
D) have the alkene of 6 to 10 carbon atoms, or
Any mixture of aforementioned substances, depend on the various compositions of sending into the heavier petroleum naphtha in the catforming process as charging wherein accurate the composition.But the method according to this invention is suitable for C
6+The various described composition of fraction.
From C
6+The hydro carbons of fraction preferably reacts on solid catalyst under the situation of input heat in gas phase with water vapor.Exist vaporous water (steam) under the situation that is continuing the input heat on the catalyzer, to make gaseous state C
6+The fraction dealkylation, thus desired product benzene and hydrogen except carbon monoxide, carbonic acid gas and other by products, formed.
The required heat of dealkylation reaction preferably produces by the burning of feed material and air.From vapor reaction by product, especially carbon monoxide and the methane of steam dealkylation, being used for burning with air as charging also is proved to be particularly preferred.From a part of vapor reaction by product, especially carbon monoxide and the methane of steam dealkylation, be combustible, thereby can produce required heat of reaction to burn as feed material.Therefore, store heat gas, and these other untapped part of reaction product sent into suitable purposes.
Purpose ground is separated into gaseous hydrogen and vapor reaction by product, especially carbon monoxide, carbonic acid gas and methane through pressure-exchange absorption with gaseous reaction products after compression.Valuable by product hydrogen exists with gaseous state equally, and can have a mind to very much the free burial ground for the destitute be used for the burning.By comprising the pressure-exchange absorption of aforementioned compression, make hydrogen easily with the combustible vapor reaction separation of by-products that can be used as aflame charging.
The flue gas that forms in burning preferably is cooled under the situation of the feed material of heating steam dealkylation through heat exchanger.Feed material (the C of the pre-heated from heat steam dealkylation by utilizing flue gas
6+Fraction and steam), also reduced in order to keep the required temperature heat necessary to be imported of dealkylation reaction.Thereby realized the economic utilization of the energy.
C
6+Fraction and water vapor preferably in pipeline, more preferably from top to bottom, process on solid catalyst, wherein catalyzer is positioned at pipe interior.Purpose ground is with the outside heat input channel.The required heat of dealkylation reaction preferably is transported on the pipeline by electromagnetic radiation, thermal radiation and/or convection current.Real dealkylation is reflected at the pipe interior that wherein has catalyzer to carry out.Guide two kinds of reaction partner (C
6+Fraction and steam) from top to bottom by pipeline with the catalyzer filling.The required heat of dealkylation reaction produces in the pipeline outside, and the described mechanical transport of process utilizes thermal conduction and convection current that heat delivery is entered on the response location of pipe interior to pipeline thus.
The preferred solid catalyst that uses is made up of following material: porous carrier materials, especially γ-Al
2O
3, magnesium-aluminium spinel and/or Cr
2O
3, and be positioned at activeconstituents on the surfaces of carrier materials, especially have the Rh of 0.1 to 1.0 weight % adsorption concentration (Beladung) and/or have the Pd of 0.2 to 2.0 weight % adsorption concentration.
Preferably at 400 ℃ to 600 ℃, more preferably 450 ℃ to 550 ℃, preferred especially 480 ℃ to 520 ℃ temperature and 1 to 15 crust more preferably 1.2 to 10 cling to, and the pressure of preferred especially 1.5 to 8 crust are implemented steam dealkylation down.
The mol ratio of purpose ground water vapor and hydro carbons in entering reactor the time is implemented steam dealkylation 1 to 20 under the situation in preferred 2 to 15 the scope.In another embodiment of the invention, the mol ratio of water vapor and hydro carbons is implemented steam dealkylation 3 to 12 under the situation in preferred 5 to 10 the scope in the time of in entering reactor.Generally speaking, implement steam dealkylation under the situation of water molar excess, wherein the accurate ratio in different embodiments of the present invention depends on C
6+The accurate composition that heats up in a steamer.
Before steam dealkylation to C
6+Fraction implements to be used to transform diolefine and cinnamic method is proved to be favourable, wherein especially adopts the method for hydrogenation that consumes hydrogen for this reason.Before steam dealkylation to C
6+Fraction is implemented to be used to transform and the method for separating the component that contains sulphur, nitrogen and/or oxygen also is favourable, wherein especially adopts the method for hydrogenation that consumes hydrogen for this reason.By adopting method for hydrogenation, can be with C
6+The diolefine that may exist in the fraction is converted into its corresponding alkene or is ethylbenzene with styrene conversion, equally also can transform and separates the component that contains sulphur, nitrogen and/or oxygen.Thus, avoided catalyzer deactivate and significant prolongation the working time of catalyzer (Laufzeit).
The reaction product of preferred cooling steam dealkylation, and in 3 are separated, be separated into gaseous reaction products, hydro carbons and water.Reaction product from steam dealkylation not only contains desired valuable product benzene and hydrogen, but also contains reaction product and byproduct of reaction such as carbon monoxide and carbonic acid gas.In order to obtain desired valuable product, must reaction product isolated.Be separated through 3 the refrigerative reaction product is separated into the especially hydro carbons and the water of gaseous reaction products, the especially benzene of hydrogen, carbon monoxide, carbonic acid gas and methane.
Purpose ground will be at C
6+The hydrogen that forms in the steam dealkylation of fraction is completely or partially delivered in the charging of the method that consumes hydrogen.The hydrogen that produces completely or partially can be used for the method for foregoing consumption hydrogen in steam dealkylation, thereby the demand to outside hydrogen to be imported is minimized.
In another embodiment of the invention, will be at C
6+The hydrogen that forms in the steam dealkylation of fraction is sent in the method that consumes hydrogen arbitrarily as feed material in refinery, especially sends into to be used for transforming and the method for separate sulphur component or send into and utilize hydrogen to decompose in the method for hydrocarbonaceous feed.
For good productive rate from the desired reaction product benzene of steam dealkylation, before steam dealkylation with C
6+Sulphur content in the fraction is reduced to and is lower than 10ppm, preferably is lower than 3ppm, especially preferably is lower than 1ppm, is proved to be favourable.
Preferably isolate benzene from the hydro carbons of reaction product through rectifying.Preferably benzene is implemented the meticulous purification of adsorptivity with dry and removal trace components after the rectifying, wherein carry benzene through sorbent material, trace components and benzene are adsorbed on the contrary on sorbent material.By adopting the method according to this invention, can obtain benzene from reaction product by simple rectifying, and further process or put on market.Do not need complicated extraction or extracting rectifying, for example adopt method, thereby reduced cost of investment and method cost according to prior art.
C
6+Preferably being transformed in the fraction by steam dealkylation with benzene boiling point component approaching or that form azeotropic mixture.Purpose ground will be chosen wantonly from all reaction product of mainly being made up of the unconverted feed material of steam dealkylation than the more difficult ebullient of benzene of rectifying and send back in the steam dealkylation process as feed material through over hydrogenation.In another embodiment of the invention, will mainly before steam dealkylation, send C back to than the more difficult ebullient of benzene from all of rectifying by the reaction product that the unconverted feed material of steam dealkylation is formed
6+The hydrogenation process of fraction or mainly by the hydrogenation process of the fraction of hydrocarbon composition with at least 5 carbon atoms.By unconverted feed material being sent back to hydrogenation process or steam dealkylation process, realized circulation, and can not lose valuable feed material.
In another embodiment of the invention, before steam dealkylation, utilize liquid-liquid extraction from C
6+Fraction is isolated straight chain hydrocarbon, wherein straight chain hydrocarbon is sent back in the feed material of catalytic reforming.
In another embodiment of the invention, before steam dealkylation by C
6+The fraction fractionation by distillation goes out main fraction (C by the hydrocarbon composition with 8 carbon atoms
8Fraction), wherein with C
8Fraction is sent into the method that is used for obtaining p-Xylol as feed material.Preferably in separation of C
8After the fraction before steam dealkylation by C
6+Fraction is isolated benzene.Pass through separation of C
8Fraction and Separation of Benzene, C
6+Fraction mainly contains toluene now, and it changes into benzene effectively by adopting the method according to this invention.
The purpose that is proposed is to realize by the equipment of the stove that comprises the pipeline that has the combustion chamber and be positioned at the combustion chamber aspect equipment.Real steam dealkylation is to implement at the pipeline of the combustion chamber that is arranged in this stove, can produce the required heat of dealkylation reaction at this.
Be installed in the combustion chamber to the pipeline preferred vertical, and in the lower end and/or the upper end have the temperature compensation element.The lower end of vertical ducting and/or the temperature compensation element on the upper end have stoped the mechanical stress of the loss raising that can cause pipeline by the temperature difference.
Purpose ground, each pipeline has C
6+The input unit of fraction and water vapor and the take-off equipment of reaction product.
Each pipe interior is filled with catalyzer and also is proved to be favourable, and wherein catalyzer is made up of following material: porous carrier materials, especially γ-Al
2O
3, magnesium-aluminium spinel and/or Cr
2O
3, and be positioned at activeconstituents on the surfaces of carrier materials, especially have the Rh of 0.1 to 1.0 weight % adsorption concentration (Beladung) and/or have the Pd of 0.2 to 2.0 weight % adsorption concentration.
Stove preferably on wall, covering and/or having at least one burner in the bottom.This pipeline of purpose ground is suitable for 1 to 15 crust, preferred 1.2 to 10 crust, and the interior pressure of preferred especially 1.5 to 8 crust, and be applicable in the stove with the highest 1400 ℃ flame temperature.
Especially can be provided in the device that is used for the catalytic reforming hydrocarbonaceous feed by the present invention and to handle C
6+The selection at the economy of prior art of fraction.By adopting the method according to this invention and, except spendable product benzene, also producing valuable by product hydrogen according to equipment of the present invention.
Claims (35)
1. be used to handle main fraction (C by hydrocarbon composition with at least 6 carbon atoms
6+Fraction) method, this fraction are to form in the device that is used for the catalytic reforming hydrocarbonaceous feed, it is characterized in that, to this C
6+Fraction is implemented steam dealkylation, except such as two kinds of spendable product material benzene of main generation and the hydrogen reaction product of carbon monoxide and carbonic acid gas.
2. method according to claim 1 is characterized in that, described C
6+Fraction mainly contains:
A) have the aromatic hydrocarbons of 6 to 10 carbon atoms,
B) have the cyclic paraffins (naphthenic hydrocarbon) of 5 to 10 carbon atoms,
C) have the different paraffin and the positive paraffin of 5 to 10 carbon atoms,
D) have the alkene of 6 to 10 carbon atoms, or
Any mixture of aforementioned substances.
3. method according to claim 1 and 2 is characterized in that, from described C
6+The hydro carbons of fraction and water vapor react on solid catalyst under the situation of input heat in gas phase.
4. according to the described method of one of claim 1 to 3, it is characterized in that the required heat of described dealkylation reaction burns by feed material and air and produces.
5. according to the described method of one of claim 1 to 4, it is characterized in that, the gaseous reaction products of described steam dealkylation is separated into gaseous hydrogen and vapor reaction by product, especially carbon monoxide, carbonic acid gas and methane through pressure-exchange absorption after compression.
6. according to the described method of one of claim 1 to 5, it is characterized in that, will be used for and air combustion as feed material from vapor reaction by product, especially carbon monoxide and the methane of described steam dealkylation.
7. according to the described method of one of claim 1 to 6, it is characterized in that the flue gas that produces is cooled under the situation of the feed material of heating steam dealkylation through heat exchanger when burning.
8. according to the described method of one of claim 1 to 7, it is characterized in that described C
6+Fraction and water vapor in pipeline, preferably from top to bottom, process on solid catalyst, wherein this catalyzer is positioned at this pipe interior.
9. according to the described method of one of claim 1 to 8, it is characterized in that, the heat of outside is imported described pipeline.
10. method according to claim 9 is characterized in that, the required heat of described dealkylation reaction is transported on the described pipeline by electromagnetic radiation, thermal radiation and/or convection current.
11., it is characterized in that used solid catalyst is made up of following material according to the described method of one of claim 1 to 10: porous carrier materials, especially γ-Al
2O
3, magnesium-aluminium spinel and/or Cr
2O
3, and be positioned at activeconstituents on this surfaces of carrier materials, especially have the Rh of 0.1 to 1.0 weight % adsorption concentration and/or have the Pd of 0.2 to 2.0 weight % adsorption concentration.
12. according to the described method of one of claim 1 to 11, it is characterized in that,, more preferably 450 ℃ to 550 ℃, implement described steam dealkylation under preferred especially 480 ℃ to the 520 ℃ temperature at 400 ℃ to 600 ℃.
13., it is characterized in that at 1 to 15 crust, more preferably 1.2 to 10 crust are implemented described steam dealkylation under the pressure of preferred especially 1.5 to 8 crust according to the described method of one of claim 1 to 12.
14., it is characterized in that the mol ratio of water vapor and hydro carbons is implemented described steam dealkylation 1 to 20 in the time of in entering reactor under the situation in preferred 2 to 15 the scope according to the described method of one of claim 1 to 13.
15., it is characterized in that the mol ratio of water vapor and hydro carbons is implemented described steam dealkylation 3 to 12 in the time of in entering reactor under the situation in preferred 5 to 10 the scope according to the described method of one of claim 1 to 14.
16. according to the described method of one of claim 1 to 15, it is characterized in that, before described steam dealkylation to described C
6+Fraction implements to be used to transform diolefine and cinnamic method, especially adopts the method for hydrogenation that consumes hydrogen for this reason.
17. according to the described method of one of claim 1 to 16, it is characterized in that, before described steam dealkylation to described C
6+The method that fraction enforcement is used to transform and separate the component that contains sulphur, nitrogen and/or oxygen especially adopts the method for hydrogenation that consumes hydrogen for this reason.
18., it is characterized in that according to the described method of one of claim 1 to 17, cool off the reaction product of described steam dealkylation, and in 3 are separated, be separated into gaseous reaction products, hydro carbons and water.
19. according to claim 16 or 17 described methods, it is characterized in that, will be at described C
6+The hydrogen that forms in the steam dealkylation of fraction is completely or partially delivered in the charging according to the method for claim 16 or 17 described consumption hydrogen.
20. according to the described method of one of claim 1 to 19, it is characterized in that, will be at described C
6+The hydrogen that forms in the steam dealkylation of fraction is sent in the method that consumes hydrogen arbitrarily as feed material in refinery, especially sends into to be used for transforming and the method for separate sulphur component or send into and utilize hydrogen to decompose in the method for hydrocarbonaceous feed.
21. according to the described method of one of claim 1 to 20, it is characterized in that, before described steam dealkylation with described C
6+Sulphur content in the fraction is reduced to and is lower than 10ppm, preferably is lower than 3ppm, especially preferably is lower than 1ppm.
22. according to the described method of one of claim 1 to 21, it is characterized in that, isolate benzene from the hydro carbons of reaction product through rectifying.
23. method according to claim 22 is characterized in that, after the rectifying benzene is implemented the meticulous purification of adsorptivity with dry and removal trace components, carries benzene through sorbent material, this trace components of absorption on this sorbent material.
24. according to the described method of one of claim 1 to 23, it is characterized in that, with described C
6+Transform by described steam dealkylation with benzene boiling point component approaching or that form azeotropic mixture in the fraction.
25. according to the described method of one of claim 22 to 24, it is characterized in that, will choose wantonly from all reaction product of mainly forming than the more difficult ebullient of benzene of rectifying and send back in the described steam dealkylation process as feed material through over hydrogenation by the unconverted feed material of described steam dealkylation.
26. according to the described method of one of claim 22 to 24, it is characterized in that, will mainly before described steam dealkylation, send described C back to than the more difficult ebullient of benzene from all of rectifying by the reaction product that the unconverted feed material of described steam dealkylation is formed
6+The hydrogenation process of fraction or mainly by the hydrogenation process of the fraction of hydrocarbon composition with at least 5 carbon atoms.
27. according to the described method of one of claim 1 to 26, it is characterized in that, before described steam dealkylation, utilize liquid-liquid extraction from described C
6+Fraction is isolated straight chain hydrocarbon, this straight chain hydrocarbon is sent back in the feed material of catalytic reforming.
28. according to the described method of one of claim 1 to 27, it is characterized in that, before described steam dealkylation by described C
6+The fraction fractionation by distillation goes out main fraction (C by the hydrocarbon composition with 8 carbon atoms
8Fraction), wherein with this C
8Fraction is sent into the method that is used for obtaining p-Xylol as feed material.
29. method according to claim 28 is characterized in that, is separating described C
8After the fraction before described steam dealkylation by described C
6+Fraction is isolated benzene.
30. be used to handle main fraction (C by hydrocarbon composition with at least 6 carbon atoms
6+Fraction) equipment, this fraction are to form in the device that is used for the catalytic reforming hydrocarbonaceous feed, it is characterized in that, this equipment comprises the stove of the pipeline that has the combustion chamber and be positioned at this combustion chamber.
31. equipment according to claim 30 is characterized in that, described pipeline vertically is installed in the described combustion chamber, and in the lower end and/or the upper end have the temperature compensation element.
32., it is characterized in that each described pipeline has and is used for described C according to claim 30 or 31 described equipment
6+The input unit of fraction and water vapor and the take-off equipment of reaction product.
33., it is characterized in that each described pipe interior is filled with catalyzer according to the described equipment of one of claim 30 to 32, this catalyzer is made up of following material: porous carrier materials, especially γ-Al
2O
3, magnesium-aluminium spinel and/or Cr
2O
3, and be positioned at activeconstituents on this surfaces of carrier materials, especially have the Rh of 0.1 to 1.0 weight % adsorption concentration and/or have the Pd of 0.2 to 2.0 weight % adsorption concentration.
34. according to the described equipment of one of claim 30 to 33, it is characterized in that, described stove on wall, covering and/or having at least one burner in the bottom.
35., it is characterized in that described pipeline is suitable for 1 to 15 crust according to the described equipment of one of claim 30 to 34, preferred 1.2 to 10 crust, the interior pressure of preferred especially 1.5 to 8 crust, and be applicable in the stove with the highest 1400 ℃ flame temperature.
Applications Claiming Priority (3)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DE102006038892 | 2006-08-18 | ||
| DE102006038892.5 | 2006-08-18 | ||
| DE102006058534.8 | 2006-12-12 |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN101130473A true CN101130473A (en) | 2008-02-27 |
Family
ID=39127905
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CNA2007101426209A Pending CN101130473A (en) | 2006-08-18 | 2007-08-20 | Method and apparatus for steam dealkylation in a plant for the catalytic reforming of hydrocarbons |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN101130473A (en) |
-
2007
- 2007-08-20 CN CNA2007101426209A patent/CN101130473A/en active Pending
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Application publication date: 20080227 |