CN1039046A - The method that hydrocarbon raw material is transformed - Google Patents
The method that hydrocarbon raw material is transformed Download PDFInfo
- Publication number
- CN1039046A CN1039046A CN89104264A CN89104264A CN1039046A CN 1039046 A CN1039046 A CN 1039046A CN 89104264 A CN89104264 A CN 89104264A CN 89104264 A CN89104264 A CN 89104264A CN 1039046 A CN1039046 A CN 1039046A
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- China
- Prior art keywords
- raw material
- arbitrary
- zeolite
- hydrocarbon
- temperature
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Classifications
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G25/00—Refining of hydrocarbon oils in the absence of hydrogen, with solid sorbents
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G11/00—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
- C10G11/02—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils characterised by the catalyst used
- C10G11/04—Oxides
- C10G11/05—Crystalline alumino-silicates, e.g. molecular sieves
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- Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Crystallography & Structural Chemistry (AREA)
- Catalysts (AREA)
- Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
Abstract
The method that the hydrocarbon raw material that makes full boiling point be at most 330 ℃ transforms, this method are included in and make this hydrocarbon raw material under the temperature that is higher than 500 ℃ is that the zeolite catalyst of 0.3～0.7 millimicron zeolite contacts with a kind of aperture of containing, and is less than 10 seconds duration of contact.
Description
The present invention relates to a kind of method that hydrocarbon raw material is transformed.
US-A-4,390, described a kind of method that hydrocarbon raw material is upgrade in 413, this method is hydrocarbon raw material to be lower than under the condition of the pressure of 14 crust, 260～427 ℃ temperature and the space velocity of 0.1～15 1/lh contact with the catalyzer that contains ZSM-5 in fixed-bed reactor.The content of nitrogenous compound is converted into nitrogen and must be less than 5ppmw in the raw material.Though illustrational raw material is a gas oil, the raw material that is suitable for comprises that also boiling range is 82～649 ℃ a hydrocarbon.Product comprises alkene such as propylene and butylene.It is desirable making alkene like this, because the valuable often product of the alkene of gained.The shortcoming of this method is that raw material must be through strict denitrogenation.This is necessary, because nitrogenously in the raw material many can make rapid catalyst deactivation.
Surprisingly, under the requirement to the nitrogen content of raw material is not so strict condition, use certain zeolite catalyst, make raw material at high temperature carry out contacting of short period of time, can obtain the alkene of high yield with catalyzer.
Therefore, the invention provides the method that a kind of hydrocarbon raw material that makes full boiling point be at most 330 ℃ transforms, this method is included in and makes this hydrocarbon raw material under the temperature that is higher than 500 ℃ is that the zeolite catalyst of the zeolite of 0.3～0.7 millimicron (being preferably 0.5～0.7 millimicron) contacts with a kind of aperture of containing, and is less than 10 seconds duration of contact.Be preferably 0.1 second minimum duration of contact.Be to obtain good result under 0.2～6 second the situation in duration of contact.
Wonderful characteristics of the present invention can be by US-A-4, and 100,218 obtain further instruction, this patent specification describe a kind of use the aperture less than 0.7 millimicron zeolite catalyst by olefin production LPG(liquefied petroleum gas (LPG), C
3 4Stable hydrocarbon) and the method for gasoline.As everyone knows, this zeolite catalyst has that to make conversion of olefines be the catalytic activity of stable hydrocarbon and aromatic hydrocarbon, thus present method to make alkene and generate less gaseous saturated hydrocarbon product be wonderful.
Temperature of reaction is 500～900 ℃, is preferably 550～800 ℃.
The aperture that this zeolite catalyst can contain one or more is 0.3～0.7 millimicron a zeolite.This catalyzer also should contain a kind of refractory oxide as tackiness agent.The refractory oxide that is fit to has aluminum oxide, silicon-dioxide, sial, magnesium oxide, titanium dioxide, zirconium white and composition thereof, is good with aluminum oxide especially.The weight ratio of refractory oxide and zeolite is preferably (10: 90)～(90: 10) and is preferably (50: 50)～(85: 15).The contained zeolite of this zeolite catalyst preferably basically just the aperture be 0.3～0.7 millimicron zeolite.Be to use down at 500～750 ℃ to contain the zeolite catalyst that the aperture is 0.5～0.7 millimicron a zeolite in of the present invention giving an example.
This term of zeolite used in this specification sheets not only includes only crystalline aluminosilicate.It also comprises crystalline silica (silicite), aluminosilicophosphate (SAPO), silicic acid chromium, silicic acid gallium, ferric metasilicate, aluminum phosphate (ALPO), titanoaluminosilicatmolecular (TASO), borosilicate, titanium aluminate or phosphate (TAPO) and iron aluminosilicate.Can be used for method of the present invention and the aperture be that the example of 0.3～0.7 millimicron zeolite has US-A-4,440, SAPO-4 described in 871 and SAPO-4 and SAPO-11, US-A-4,310, ALPO-11 described in 440, US-A-4,500, TAPO-11 described in 651, EP-A-229, the TASO-45 described in 295, for example US-A-4,254, borosilicate described in 297, pure aluminium silicate such as erionite, ferrierite, Q(fhefa) zeolite and ZSM-5, the ZSM type zeolite of ZSM-11, ZSM-12, ZSM-35, ZSM-23 and ZSM-38 and so on.Preferably zeolite system is selected from metal silicate with ZSM-5 structure, ferrierite, erionite and composition thereof.The crystal metal silicate with ZSM-5 structure that is suitable for is just like GB-B-2, the pure aluminium silicate described in 110,559, silicic acid gallium, ferric metasilicate, scandium silicate, silicic acid rhodium and (or) silicic acid chromium.
The alkalimetal oxide that in preparing resulting zeolite, contains a great deal of usually.The most handy technical known method such as ion exchange method are removed these basic metal, then also can calcine, to make the zeolite that is with hydrogen bonding state (in ifs hydrogen form).The zeolite that is used for present method preferably is and hydrogen bonded state basically.
The pressure that present method adopted can change within a large range.But preferably this pressure can make raw material be in gas phase state basically or be gas phase state by contacting with catalyzer under main temperature.Be convenient to reach the duration of contact of the weak point of expectation like that.Therefore, present method should adopt lower pressure.This is favourable, because so just do not need to use expensive compressor and high pressure vessel and other equipment.The pressure range that is fit to is 1～10 crust.Employing is lower than 1 atmospheric pressure and also is fine, but should not do like this.Adopting normal pressure is being favourable on mist.In conversion process, may also have other gaseous substances to exist, as water vapor and (or) nitrogen.
Present method is preferably in the moving-bed and implements.Beds can move up or down.When beds moved up, this method was similar a bit to FCC process.
In present method implementation process, can on catalyzer, form some charcoal Jiao.Therefore, must make catalyst regeneration.The regenerated method is to be preferably in catalyzer to contact back oxidizing gas (as air) processing catalyzer with raw material.Preferably adopt the cyclic regeneration method be similar in the FCC process to be adopted.
If the burnt speed that forms of charcoal is not too fast, can adopt such method, even in the reaction process residence time of granules of catalyst in reaction zone be longer than the residence time of raw material in reaction zone.Certainly, should be less than 10 seconds the duration of contact of raw material and catalyzer.Duration of contact is general consistent with the residence time of raw material.The residence time of catalyzer is preferably 1～20 times of the residence time of raw material.
Though the requirement to the weight ratio of catalyzer and raw material is not strict, per 1 kilogram of raw material should use the catalyzer more than 1～150 or 150 kilogram.The weight ratio of catalyzer and raw material is preferably (20～120): 1.
The raw material that present method will transform contains the hydrocarbon that full boiling point is at most 330 ℃.According to these characteristics, low-density oil cut such as raw gasline and kerosene include interior.The initial boiling point of raw material is preferably-45 ℃.The raw material that is fit to comprises C
3-4Hydrocarbon (for example LPG(liquefied petroleum gas (LPG))), raw gasline, gasoline fraction, kerosene(oil)fraction and composition thereof.
With US-A-4,390,413 method is compared, and one of advantage of present method is can use the higher raw material of nitrogen content and can not influence activity of such catalysts basically.The nitrogen content of the raw material that is suitable for change etc. for nitrogen can be greater than 25ppmw.Even can reach 100～1000ppmw.
The present invention is further illustrated with embodiment below.
Embodiment 1
In a series of tests, use C with following composition
5 7Hydrocarbon mixture transforms:
Iso-pentane 25.7%(weight)
Skellysolve A 26.3%(weight)
Isohexane 0.3%(weight)
Normal hexane 23.4%(weight)
Isoheptane 0.8%(weight)
Normal heptane 23.5%(weight)
As can be seen, the boiling point of the compound that boiling point is the highest is 98.5 ℃.
Test is carried out in a downflow reactor, and raw material and median size are 74 microns same the flowing downward of granules of catalyst in this reactor.Used catalyzer contain in alumina substrate, be with the ZSM-5(ZSM-5 of hydrogen bonding state and the weight ratio of aluminum oxide be 1: 3).All tests are all carried out under normal pressure.Concrete reaction conditions and test-results all are shown in the following table 1.
Symbol "=" expression ethylenically unsaturated hydrocarbons in the table, " C
+
5" expression contains the hydrocarbon product that does not belong to n-paraffin or isoparaffin of 5 or 5 above carbon atoms.
Table 1
The experiment number
Temperature 1234
℃ 400 500 500 550
The catalyst/oil ratio, kg/kg 8.0 5.8 30.1 34.9
Duration of contact, s 2.0 2.0 2.0 2.0
Product %wt
H
20.0 0.1 0.1 0.2
C
10.0 0.2 0.3 1.2
C
20.2 2.4 3.3 7.5
C
31.9 7.0 10.6 14.1
C
42.3 4.6 7.0 7.8
i-C
526.3 24.9 24.5 22.7
n-C
525.8 23.9 22.7 22.1
i-C
60.4 0.3 0.3 0.2
n-C
620.6 18.1 14.7 12.3
i-C
70.8 0.5 0.5 0.3
n-C
720.0 16.3 12.9 7.2
C
+
50.9 0.8 1.1 1.4
0.8 0.9 2.0 3.0
Coke on the catalyzer
Degree of unsaturation
C
＝
2/C
21.7 1.8 1.9 1.7
C
≠
3/C
30.8 1.1 1.0 1.5
C
≠
4/C
40.5 1.3 1.1 1.9
Can find out significantly that from above result n-paraffin preferentially obtains cracking and produces the gaseous product contain a large amount of alkene, especially be higher than under 500 ℃ the temperature condition all the more so.More than 500 ℃, C
3And C
4The ratio of alkene and paraffinic hydrocarbons improves significantly, and the total conversion rate that is converted into light alkene improves.The ratio result that the ratio of different in the liquid product of gained/n-paraffin is higher than in the raw mix also makes the octane value raising of liquid product gasoline thereby its quality is improved.
Embodiment 2
Further with C with following component
5 10Hydrocarbon mixture transforms (numeral is the weight percent of charging) as raw material:
Paraffinic hydrocarbons 55.9
Naphthenic hydrocarbon 32.9
Aromatic hydrocarbon 11.3
The IBP(initial boiling point) 50 ℃
The FBP(full boiling point) 199 ℃
50% 119℃
Utilize embodiment 1 described reactor and catalyzer under normal pressure, to test.Concrete reaction conditions and test-results are shown in Table 2.
Symbol "=" expression ethylenically unsaturated hydrocarbons in the table.
Table 2
Reaction conditions:
Temperature of reaction, ℃ 580
The catalyst/oil ratio, g/g 112
Duration of contact, s 1.9
Product accounts for the percentage ratio of charging
C
11.4
C
21.7
C
＝
27.4
C
34.0
C
＝
316.5
C
42.3
C
＝
48.0
C
5-221℃ 50.5
221-370℃ 0.8
Coke 7.0
Can see the rate of output high mainly be C
2-4Olefin product.
Claims (15)
1, the method that transforms of a kind of hydrocarbon raw material that makes full boiling point be at most 330 ℃, this method are included in and make this hydrocarbon raw material under the temperature that is higher than 550 ℃ is that the zeolite catalyst of 0.3～0.7 millimicron zeolite contacts with a kind of aperture of containing, and is less than 10 seconds duration of contact.
2, a kind of method of claim 1, wherein be 0.2～6 second the duration of contact of raw material and zeolite catalyst.
3, claim 1 or a kind of method of 2, wherein temperature is 500～900 ℃.
4, a kind of method of claim 3, wherein temperature is 550～800 ℃.
5, a kind of method of arbitrary claim in the claim 1～4, wherein the contained zeolite of zeolite catalyst basically just the aperture be 0.3～0.7 millimicron zeolite.
6, a kind of method of arbitrary claim in the above claim, the aperture of its mesolite is 0.5～0.7 millimicron, temperature is to nearly 750 ℃.
7, a kind of method of arbitrary claim in the claim 1～6, its mesolite system is selected from crystal metal silicate with ZSM-5 structure, ferrierite, erionite and composition thereof.
8, the method for arbitrary claim in the claim 1～7, wherein zeolite is and hydrogen bonded state basically.
9, a kind of method of arbitrary claim in the claim 1～8, wherein pressure is 1～10 crust.
10, a kind of method of arbitrary claim in the claim 1～9, wherein the weight ratio of catalyzer and raw material is (1～150): 1, be preferably (20～120): 1.
11, a kind of method of arbitrary claim in the claim 1～10, this method is to implement in the moving-bed of catalyzer.
12, a kind of method of arbitrary claim in the claim 1～11, wherein the initial boiling point of raw material is at least-45 ℃.
13, a kind of method of claim 12, wherein raw material contains C
3 4Hydrocarbon, raw gasline, gasoline, kerosene or its mixture.
14, a kind of method of claim 1, basically as previously described in the embodiment.
15, use hydrocarbon product or its cut of the method acquisition of the arbitrary claim in the claim of front.
Applications Claiming Priority (4)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| GB888814293A GB8814293D0 (en) | 1988-06-16 | 1988-06-16 | Process for conversion of hydrocarbonaceous feedstock |
| GB8814293.0 | 1988-06-16 | ||
| GB8904409.3 | 1989-02-27 | ||
| GB898904409A GB8904409D0 (en) | 1989-02-27 | 1989-02-27 | Process for the conversion of a hydrocarbonaceous feedstock |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN1039046A true CN1039046A (en) | 1990-01-24 |
| CN1021913C CN1021913C (en) | 1993-08-25 |
Family
ID=26294030
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN89104264A Expired - Fee Related CN1021913C (en) | 1988-06-16 | 1989-06-14 | Process for conversion of phdrocarbonaceous feedstock |
Country Status (10)
| Country | Link |
|---|---|
| EP (1) | EP0347003B1 (en) |
| JP (1) | JPH0245593A (en) |
| KR (1) | KR910001002A (en) |
| CN (1) | CN1021913C (en) |
| AU (1) | AU614626B2 (en) |
| BR (1) | BR8902859A (en) |
| DE (1) | DE68926408T2 (en) |
| ES (1) | ES2087073T3 (en) |
| PH (1) | PH25773A (en) |
| RU (1) | RU2002794C1 (en) |
Families Citing this family (21)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB8828206D0 (en) * | 1988-12-02 | 1989-01-05 | Shell Int Research | Process for conversion of hydrocarbonaceous feedstock |
| GB8904408D0 (en) * | 1989-02-27 | 1989-04-12 | Shell Int Research | Process for the conversion of a hydrocarbonaceous feedstock |
| GB8908081D0 (en) * | 1989-04-11 | 1989-05-24 | Shell Int Research | Process for the conversion of a hydrocarbonaceous feedstock |
| US4969987A (en) * | 1989-11-29 | 1990-11-13 | Mobil Oil Corporation | Integrated process for production of gasoline and ether |
| US5100533A (en) * | 1989-11-29 | 1992-03-31 | Mobil Oil Corporation | Process for production of iso-olefin and ether |
| US5100534A (en) * | 1989-11-29 | 1992-03-31 | Mobil Oil Corporation | Hydrocarbon cracking and reforming process |
| GB9114390D0 (en) * | 1991-07-03 | 1991-08-21 | Shell Int Research | Hydrocarbon conversion process and catalyst composition |
| EP0920911A1 (en) | 1997-12-05 | 1999-06-09 | Fina Research S.A. | Production of catalysts for olefin conversion |
| US6069287A (en) * | 1998-05-05 | 2000-05-30 | Exxon Research And Engineering Co. | Process for selectively producing light olefins in a fluid catalytic cracking process |
| US6803494B1 (en) | 1998-05-05 | 2004-10-12 | Exxonmobil Chemical Patents Inc. | Process for selectively producing propylene in a fluid catalytic cracking process |
| US6388152B1 (en) | 1998-05-05 | 2002-05-14 | Exxonmobil Chemical Patents Inc. | Process for producing polypropylene from C3 olefins selectively produced in a fluid catalytic cracking process |
| US6455750B1 (en) | 1998-05-05 | 2002-09-24 | Exxonmobil Chemical Patents Inc. | Process for selectively producing light olefins |
| US6093867A (en) * | 1998-05-05 | 2000-07-25 | Exxon Research And Engineering Company | Process for selectively producing C3 olefins in a fluid catalytic cracking process |
| US6118035A (en) | 1998-05-05 | 2000-09-12 | Exxon Research And Engineering Co. | Process for selectively producing light olefins in a fluid catalytic cracking process from a naphtha/steam feed |
| US6313366B1 (en) | 1998-05-05 | 2001-11-06 | Exxonmobile Chemical Patents, Inc. | Process for selectively producing C3 olefins in a fluid catalytic cracking process |
| US6602403B1 (en) | 1998-05-05 | 2003-08-05 | Exxonmobil Chemical Patents Inc. | Process for selectively producing high octane naphtha |
| US6315890B1 (en) | 1998-05-05 | 2001-11-13 | Exxonmobil Chemical Patents Inc. | Naphtha cracking and hydroprocessing process for low emissions, high octane fuels |
| US6339180B1 (en) | 1998-05-05 | 2002-01-15 | Exxonmobil Chemical Patents, Inc. | Process for producing polypropylene from C3 olefins selectively produced in a fluid catalytic cracking process |
| US6106697A (en) | 1998-05-05 | 2000-08-22 | Exxon Research And Engineering Company | Two stage fluid catalytic cracking process for selectively producing b. C.su2 to C4 olefins |
| US6222087B1 (en) | 1999-07-12 | 2001-04-24 | Mobil Oil Corporation | Catalytic production of light olefins rich in propylene |
| US6835863B2 (en) | 1999-07-12 | 2004-12-28 | Exxonmobil Oil Corporation | Catalytic production of light olefins from naphtha feed |
Family Cites Families (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3140322A (en) * | 1958-08-14 | 1964-07-07 | Socony Mobil Oil Co Inc | Selective catalytic conversion |
| US3856659A (en) * | 1972-12-19 | 1974-12-24 | Mobil Oil Corp | Multiple reactor fcc system relying upon a dual cracking catalyst composition |
| US3886060A (en) * | 1973-04-30 | 1975-05-27 | Mobil Oil Corp | Method for catalytic cracking of residual oils |
| US4218344A (en) * | 1975-12-19 | 1980-08-19 | Standard Oil Company (Indiana) | Catalytic cracking with reduced emission of noxious gases |
| US4100218A (en) * | 1977-05-31 | 1978-07-11 | Mobil Oil Corporation | Ethane conversion process |
| US4390413A (en) * | 1979-12-26 | 1983-06-28 | Chevron Research Company | Hydrocarbon upgrading process |
| US4310440A (en) * | 1980-07-07 | 1982-01-12 | Union Carbide Corporation | Crystalline metallophosphate compositions |
| GB8814292D0 (en) * | 1988-06-16 | 1988-07-20 | Shell Int Research | Process for conversion of hydrocarbonaceous feedstock |
-
1989
- 1989-06-14 AU AU36394/89A patent/AU614626B2/en not_active Ceased
- 1989-06-14 ES ES89201558T patent/ES2087073T3/en not_active Expired - Lifetime
- 1989-06-14 PH PH38786A patent/PH25773A/en unknown
- 1989-06-14 CN CN89104264A patent/CN1021913C/en not_active Expired - Fee Related
- 1989-06-14 BR BR898902859A patent/BR8902859A/en not_active IP Right Cessation
- 1989-06-14 DE DE68926408T patent/DE68926408T2/en not_active Revoked
- 1989-06-14 KR KR1019890008211A patent/KR910001002A/en not_active Application Discontinuation
- 1989-06-14 EP EP89201558A patent/EP0347003B1/en not_active Revoked
- 1989-06-14 JP JP1149783A patent/JPH0245593A/en active Pending
- 1989-06-14 RU SU894614344A patent/RU2002794C1/en active
Also Published As
| Publication number | Publication date |
|---|---|
| CN1021913C (en) | 1993-08-25 |
| EP0347003B1 (en) | 1996-05-08 |
| AU614626B2 (en) | 1991-09-05 |
| PH25773A (en) | 1991-10-18 |
| DE68926408T2 (en) | 1996-10-31 |
| JPH0245593A (en) | 1990-02-15 |
| RU2002794C1 (en) | 1993-11-15 |
| BR8902859A (en) | 1990-02-01 |
| ES2087073T3 (en) | 1996-07-16 |
| EP0347003A1 (en) | 1989-12-20 |
| KR910001002A (en) | 1991-01-30 |
| AU3639489A (en) | 1989-12-21 |
| DE68926408D1 (en) | 1996-06-13 |
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