CN101165018B - Method for producing ethylene and propylene - Google Patents
Method for producing ethylene and propylene Download PDFInfo
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- CN101165018B CN101165018B CN200610117344A CN200610117344A CN101165018B CN 101165018 B CN101165018 B CN 101165018B CN 200610117344 A CN200610117344 A CN 200610117344A CN 200610117344 A CN200610117344 A CN 200610117344A CN 101165018 B CN101165018 B CN 101165018B
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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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- 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
- Y02P20/584—Recycling of catalysts
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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
- Y02P30/00—Technologies relating to oil refining and petrochemical industry
- Y02P30/20—Technologies relating to oil refining and petrochemical industry using bio-feedstock
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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
- Y02P30/00—Technologies relating to oil refining and petrochemical industry
- Y02P30/40—Ethylene production
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Abstract
The present invention relates to ethylene and propylene producing process with high selectivity and high yield. The production process adopts methanol and/or dimethyl ether as material, and at least one selected from water, C2-C5 alcohol, C2-C10 ether, C4+ hydrocarbon and C6-C12 arene as the terminator; and includes the following steps: 1. reaction of material and terminator in first fluidized bedreactor through contacting with catalyst I to produce effluent I containing ethylene, propylene and C4 and C4+ hydrocarbons; and treating the effluent I in a post step; 2. regenerating the catalyst II to be regenerated from the first fluidized bed reactor through contacting with the regenerating gas in the regenerating reactor; 3. deactivating the regenerated catalyst III from the regenerating reactor through contact with deactivator in the second fluidized bed reactor; and 4. returning the deactivated catalyst IV to the first fluidized bed reactor. The production process may be applied in industrial production.
Description
Technical field
The present invention relates to the production method of a kind of ethene and propylene, particularly regenerated catalyst is carried out Passivation Treatment and reaction product termination reaction, realize that oxygenatedchemicals such as methyl alcohol or dimethyl ether catalysis efficiently are converted into the method for ethene and propylene about a kind of employing regenerated catalyst Passivation Treatment system and reaction product termination tech.
Background technology
Petrochemical complex is a mainstay industry important in the national economy, for industry, agricultural, departments such as traffic and national defence provide a large amount of industrial chemicals, is one of related and branch of industry that drive property is stronger in the national economy.Propylene and ethene then are to constitute modern petrochemical complex of paramount importance two big basic materials.
Large derived product of ethene mainly contains polyethylene, oxyethane, ethylene glycol, polyvinyl chloride, vinylbenzene, vinyl acetate between to for plastic etc.The size of ethylene yield is to weigh the sign of a national petrochemical industry and even national economy development degree.Propylene is mainly used in produces polypropylene, isopropyl benzene, oxo-alcohols, vinyl cyanide, propylene oxide, vinylformic acid, Virahol etc., and wherein polypropylene accounts for the over half of world's propylene demand.At present, 67% propylene is produced the byproduct of ethene from steam cracking in the world, and 30% produces the byproduct of vapour, diesel oil from refinery catalytic cracking (FCC), and a small amount of (about 3%) is obtained by dehydrogenating propane and ethene-butylene metathesis reaction.Estimate that following ethene and propylene demand growth speed are faster than supply.
Higher in view of the growth rate of demand of ethene and propylene, and traditional production model presents the pressure of " supply falls short of demand ", so make-up ethylene and propylene demand need be by means of other various increasing output of ethylene propylene technology.
All the time; coal or Sweet natural gas preparing synthetic gas, synthesising gas systeming carbinol and alkene isolation technique have had the mass-producing mature experience; but the process by methanol to olefins is breakpoint and the difficult point of synthetic gas to this industrial chain of alkene, and this solution of key technology can be for providing a new raw material route by non-oil resource production basic organic ethene, propylene.Especially in the last few years, it is high that the demand of ethene and propylene continues, and under the deficient day by day situation of petroleum resources.How to hew out a non-oil resource and produce the Coal Chemical Industry variation route of propylene, for greatly alleviating China's oil situation in short supply, promote the great-leap-forward development of the heavy chemical industry of China and the structural adjustment of raw material route, have important strategic meaning and society, economic benefit.
Document CN1166478A, disclose a kind of method of being produced low-carbon alkenes such as ethene, propylene by methyl alcohol or dme, this method is catalyzer with the aluminium phosphate molecular sieve, adopts the ciculation fluidized formula processing method of upstriker dense bed, in 500～570 ℃ of preferred temperature of reaction, air speed 2～6 hours
-1And under 0.01～0.05MPa condition, make methyl alcohol or dme cracking produce low-carbon alkenes such as ethene, propylene.The low technical disadvantages of this method purpose product selectivity.
Document CN1356299A discloses a kind of processing method and system thereof that produces low-carbon alkene by methyl alcohol or dme.This process using silicoaluminophosphamolecular molecular sieves (SAPO-34) is as catalyzer, utilize the ultrashort contact reactor of gas-solid cocurrent flow descending formula fluidized-bed, catalyzer contacts in the ultrashort contact reactor of gas-solid cocurrent flow descending formula fluidized-bed with raw material, the reactant flow direction is descending; Catalyzer and reaction product go out to enter the gas-solid quick disconnector that is arranged on this reactor lower part behind the reactor and carry out sharp separation; Isolated catalyzer enters charcoal regeneration in the revivifier, and catalyzer is cyclic regeneration in system, and reaction cycle is carried out.This technology dme or conversion of methanol are greater than 98%.But there is the low technical disadvantages of ethylene, propylene selectivity equally in this method.
Summary of the invention
Technical problem to be solved by this invention is to have the low and low problem of selectivity of purpose product ethylene, propylene yield in the technical literature in the past, and a kind of new ethene and the production method of propylene are provided.This method has purpose product ethylene, propylene yield height, the advantage that selectivity is good.
In order to solve the problems of the technologies described above, the technical solution used in the present invention is as follows: the production method of a kind of ethene, propylene may further comprise the steps: be raw material to be selected from least a in methyl alcohol, the dme (a), to be selected from water, C
2～C
5Alcohol or C
4At least a in the above hydro carbons is terminator, raw material at first enters from first fluidized bed reactor bottom, terminator enters from first class bed bioreactor top, raw material and terminator and catalyst I contact reacts generate the effluent I that contains ethene, propylene and carbon four above hydrocarbon, and effluent I and unreacted material are discharged from first class bed bioreactor top and entered follow-up workshop section; (b) the reclaimable catalyst II in the first class bed bioreactor enters revivifier regeneration gas interior and from regenerator bottoms and contacts regeneration, and regenerated flue gas is discharged from revivifier top; (c) III of regenerated catalyst from revivifier enters second fluidized-bed reactor, and the passivator of regenerated catalyst III generation carbonaceous sediment contacts with making; (d) returning the first class bed bioreactor from the catalyst I V after the second fluidized-bed reactor passivation reacts; Wherein, catalyzer is selected from least a or its composite molecular screen in SAPO-34 molecular sieve and the ZSM-5 molecular sieve.
The temperature of reaction of first class bed bioreactor is 200～600 ℃ in the technique scheme, and reaction pressure is 0.01～1.5MPa, and be 0.1～20 second duration of contact, and catalyzer is 0.1～50 with the raw material weight ratio.First fluidized bed reactor reaction temperature preferable range is 300～550 ℃, and the reaction pressure preferable range is 0.05～1.0MPa, and duration of contact, preferable range was 0.2～10 second, and catalyzer is 0.2～10 with raw material weight than preferable range.The second fluidized-bed reactor temperature of reaction is 100～650 ℃, and reaction pressure is 0.01～1.0MPa.The first class bed bioreactor is selected from bubbling fluidized bed, turbulent fluidized bed, fast fluidized bed or riser reactor.First class bed bioreactor preferred version is selected from fast fluidized bed.In second fluidized-bed reactor on the catalyzer carbonaceous sediment weight content be 2～12%.
Studies show that in a large number, in oxygenatedchemicals such as methyl alcohol or dimethyl ether catalysis conversion process, the existence of an amount of coke is favourable to the selectivity that improves ethylene, propylene among catalyzer such as the SAPO-34, and the control of an amount of coke is depended merely on the coke-burning rate of regeneration system rapidly and is burnt the control of degree and be not only very difficultly by the modulation that mixes of live catalyst and decaying catalyst in the catalyzer, and the while effect is not very good; On the other hand, the process that the catalyzed reaction of methyl alcohol and dme generates ethene and propylene is the complex reaction network that a plurality of parallel consecutive reactions are coupled, and the product of primary first-order equation can carry out secondary reaction, reduces the yield of ethylene, propylene.Based on above analysis, the production method of ethene of the present invention and propylene, in its reactor assembly before regenerated catalyst enters reactor, earlier through the Passivation Treatment reactor, make activity of such catalysts remain on higher level by contacting, enter the first class bed bioreactor again through inactive catalyst then and react with passivator.In addition, consider that methyl alcohol or dimethyl ether catalysis conversion process are the rapid reaction processes, and the product of primary first-order equation can be proceeded secondary reaction and reduce ethylene, propylene purpose product, the first class bed bioreactor is selected from fast fluidized bed or riser reactor in the present technique invention for this reason, especially recommend to adopt fast fluidized bed reactor, while is in the injection of the upper end of fluidized-bed reactor or spray into the timely termination reaction of terminator, reduce the generation of secondary reaction, improved the effective selectivity and the yield of ethylene, propylene.
Adopt technical scheme of the present invention, with the SAPO-34 molecular sieve is catalyzer, methyl alcohol or dme are raw material, ethanol is terminator, first fluidized bed reactor reaction condition is: 300～550 ℃ of temperature of reaction, pressure 0.05～1.0MPa, 0.2～10 second duration of contact, catalyzer is 0.2～10 with the raw material weight ratio.The second fluidized-bed reactor reaction conditions is: 100～550 ℃ of temperature of reaction, pressure 0.01～1.0MPa, under 0.1～15 second duration of contact condition, ethene and propylene diene yield can be greater than 80%, feed stock conversion can reach 100%, has obtained better technical effect.
Description of drawings
Fig. 1 is used for the device synoptic diagram that oxygenatedchemicals is produced ethene and propylene for the present invention.
1 is fluidized-bed reactor I among Fig. 1, the 2nd, and revivifier, the 3rd, fluidized-bed reactor II, the 4th, regenerator sloped tube a, the 5th, inclined tube to be generated, the 6th, regenerator sloped tube b, the 7th, feed(raw material)inlet, the 8th, passivator inlet, the 9th, revivifier inlet, the 10th, regenerated flue gas, the 11st, reaction mixture outlet; The 12nd, the terminator intake.
Oxygen-containing compound material enters fluidized-bed reactor I1 haptoreaction by inlet device 7 among Fig. 1 from the bottom, the terminator intake 12 of terminator by fluidized-bed reactor I top injects or sprays into, in the mixture effect of fluidized-bed reactor I top and reaction mixture gas and catalyst, stop secondary response. Reactant mixture is after cyclone separator separates, and gaseous product is introduced subsequent treatment workshop section through the reactant mixture outlet 11 at fluidized-bed reactor I top. Reclaimable catalyst in fluidized-bed reactor I enters regenerator 2 through inclined tube 5 to be generated, the good catalyst of regeneration in the regenerator 2 enters fluidized-bed reactor II through regenerator sloped tube a, passivator enters fluidized-bed reactor II through passivator entrance 8 and contacts with reclaimable catalyst, make catalyst produce carbonaceous sediment (coke), catalyst after passivation returns fluidized-bed reactor I haptoreaction through the regenerator sloped tube b of fluidized-bed reactor I again, and this process is carried out continuously.
Haptoreaction, this process is carried out continuously.
The invention will be further elaborated below by embodiment, but be not limited only to present embodiment.
Embodiment
[embodiment 1]
[embodiment 2]
[embodiment 3]
[embodiment 4]
[embodiment 5]
[embodiment 6]
Accompanying drawing 1 shown device is adopted in test, with ZSM-5 and SAPO-34 composite molecular screen is catalyzer, ZSM-5 accounts for 10% in the catalyzer, SAPO-34 accounts for 80%, methyl alcohol and dme are raw material, wherein the weight ratio of methyl alcohol and dme is 2: 1, the FCC raw gasline is a terminator, butene-2 (83%) and normal butane (17%) hydrocarbon mixture are passivator, and the weight ratio of raw material and terminator is 15: 1,150 ℃ of terminator feed entrance temperature, first fluidized bed reactor reaction condition is: 500 ℃ of temperature of reaction, reaction pressure 0.2MPa, 8 seconds duration of contact, catalyzer is 1 with the raw material weight ratio.The second fluidized-bed reactor reaction conditions is: 500 ℃ of temperature of reaction, and pressure 0.3MPa, controlling the second fluid bed reactor catalysis agent carbon deposition quantity is 6%, its reaction result is: yield of ethene 33%, propene yield 40%.
[embodiment 7]
Accompanying drawing 1 shown device is adopted in test, with ZSM-5 and SAPO-34 composite molecular screen is catalyzer, ZSM-5 accounts for 5% in the catalyzer, SAPO-34 accounts for 80%, methyl alcohol and dme are raw material, wherein the weight ratio of methyl alcohol and dme is 5: 1, heavy gas oil is terminator, butene-2 (83%) and normal butane (17%) hydrocarbon mixture are passivator, and the weight ratio of raw material and terminator is 50: 1,40 ℃ of terminator feed entrance temperature, first fluidized bed reactor reaction condition is: 510 ℃ of temperature of reaction, reaction pressure 0.4MPa, 5 seconds duration of contact, catalyzer is 0.8 with the raw material weight ratio.The second fluidized-bed reactor reaction conditions is: 600 ℃ of temperature of reaction, and pressure 0.5MPa, controlling the second fluid bed reactor catalysis agent carbon deposition quantity is 8%, its reaction result is: yield of ethene 40%, propene yield 35%.
[comparative example 1]
Accompanying drawing 1 shown device is adopted in test, according to condition and the catalyzer of embodiment 1, does not just add terminator in the device, and in its reaction product, yield of ethene is 45%, and propene yield is 30%.
[comparative example 2]
Accompanying drawing 1 shown device is adopted in test, according to condition and the catalyzer of embodiment 1, does not just add second fluidized-bed reactor in the device, and regeneration rear catalyst carbon deposition quantity is 0.5%, and in its reaction product, yield of ethene is 47%, and propene yield is 32%.
[comparative example 3]
Accompanying drawing 1 shown device is adopted in test, according to condition and the catalyzer of embodiment 1, does not just add second fluidized-bed reactor in the device, and do not add terminator in the device, regeneration rear catalyst carbon deposition quantity is 0.5%, in its reaction product, yield of ethene is 42%, and propene yield is 29%.
Claims (8)
1. the production method of ethene and propylene may further comprise the steps:
(a) be raw material to be selected from least a in methyl alcohol, the dme, to be selected from water, C
2～C
5Alcohol or C
4At least a in the above hydro carbons is terminator, raw material at first enters from first fluidized bed reactor bottom, terminator enters from first class bed bioreactor top, raw material and terminator and catalyst I contact reacts generate the effluent I that contains ethene, propylene and carbon four above hydrocarbon, and effluent I and unreacted material are discharged from first class bed bioreactor top and entered follow-up workshop section;
(b) the reclaimable catalyst II in the first class bed bioreactor enters revivifier regeneration gas interior and from regenerator bottoms and contacts regeneration, and regenerated flue gas is discharged from revivifier top;
(c) III of regenerated catalyst from revivifier enters second fluidized-bed reactor, and the passivator of regenerated catalyst III generation carbonaceous sediment contacts with making;
(d) returning the first class bed bioreactor from the catalyst I V after the second fluidized-bed reactor passivation reacts;
Wherein, catalyzer is selected from least a or its composite molecular screen in SAPO-34 molecular sieve and the ZSM-5 molecular sieve.
2. according to the production method of described ethene of claim 1 and propylene, the temperature of reaction that it is characterized in that the first class bed bioreactor is 200～600 ℃, reaction pressure is 0.01～1.5MPa, and be 0.1～20 second duration of contact, and catalyzer is 0.1～50 with the raw material weight ratio.
3. according to the production method of described ethene of claim 2 and propylene, it is characterized in that first fluidized bed reactor reaction temperature is 300～550 ℃, reaction pressure is 0.05～1.0MPa, and be 0.2～10 second duration of contact, and catalyzer is 0.2～10 with the raw material weight ratio.
4. according to the production method of described ethene of claim 1 and propylene, it is characterized in that the second fluidized-bed reactor temperature of reaction is 100～650 ℃, reaction pressure is 0.01～1.0MPa.
5. according to the production method of described ethene of claim 1 and propylene, it is characterized in that the first class bed bioreactor is selected from bubbling fluidized bed, turbulent fluidized bed, fast fluidized bed or riser reactor.
6. according to the production method of described ethene of claim 5 and propylene, it is characterized in that the first class bed bioreactor is selected from fast fluidized bed.
7. according to the production method of described ethene of claim 1 and propylene, it is characterized in that in second fluidized-bed reactor that the carbonaceous sediment weight content is 2～12% on the catalyzer.
8. according to the production method of described ethene of claim 1 and propylene, the weight ratio that it is characterized in that raw material and terminator is 5～1000: 1, and the terminator feeding temperature is 10～200 ℃.
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| CN200610117344A CN101165018B (en) | 2006-10-20 | 2006-10-20 | Method for producing ethylene and propylene |
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| CN200610117344A CN101165018B (en) | 2006-10-20 | 2006-10-20 | Method for producing ethylene and propylene |
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| CN101165018B true CN101165018B (en) | 2010-05-12 |
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Families Citing this family (13)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101328103B (en) * | 2008-06-12 | 2012-06-27 | 中国石油化工股份有限公司 | Method for converting methanol or dimethyl ether into low carbon alkene |
| CN101332434B (en) * | 2008-07-08 | 2010-06-02 | 中国石油化工股份有限公司 | Processing method of low carbon olefin hydrocarbon reactor runoff catalyst produced by methanol or dimethyl ether |
| CN101333141B (en) * | 2008-07-08 | 2012-05-30 | 中国石油化工股份有限公司 | Reaction device for conversing methanol or dimethyl ether to be low carbon olefin |
| CN101333142B (en) * | 2008-07-08 | 2012-05-30 | 中国石油化工股份有限公司 | Starting method of reaction-regenerative device for preparing low carbon olefin form methanol |
| CN101811923B (en) * | 2009-02-19 | 2013-01-09 | 中国石油化工股份有限公司 | Method for producing propylene from methanol or dimethyl ether |
| CN102190540B (en) * | 2010-03-03 | 2013-09-18 | 中国石油化工股份有限公司 | Method for producing propylene |
| CN102190538B (en) * | 2010-03-03 | 2014-07-02 | 中国石油化工股份有限公司 | Method for Catalytic pyrolysis of hydrocarbons with more than 4 carbon atoms in process of preparing olefins from methanol |
| CN102463137B (en) * | 2010-11-17 | 2013-12-18 | 中国石油化工股份有限公司 | Treatment method for three-spinning recycling of catalyst in reactor for preparing alkene from methyl alcohol |
| CN102464522B (en) * | 2010-11-17 | 2015-02-11 | 中国石油化工股份有限公司 | Method for producing low-carbon olefins |
| CN102464523B (en) * | 2010-11-17 | 2014-04-23 | 中国石油化工股份有限公司 | Method for producing light olefins |
| CN102464534B (en) * | 2010-11-17 | 2014-11-26 | 中国石油化工股份有限公司 | Method for producing low-carbon olefins from methanol |
| CN102649088B (en) * | 2011-02-25 | 2014-04-23 | 中国石油化工股份有限公司 | Treatment method for catalyst escaping from reactor during preparing low-carbon alkene from methanol or dimethyl ether |
| CN104399522A (en) * | 2014-10-21 | 2015-03-11 | 贵州大学 | Catalyst for production of low carbon olefin from methanol through iodination method, and preparation method thereof |
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