CN101165019B - Method for producing ethylene and propylene - Google Patents

Method for producing ethylene and propylene Download PDF

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Publication number
CN101165019B
CN101165019B CN2006101173450A CN200610117345A CN101165019B CN 101165019 B CN101165019 B CN 101165019B CN 2006101173450 A CN2006101173450 A CN 2006101173450A CN 200610117345 A CN200610117345 A CN 200610117345A CN 101165019 B CN101165019 B CN 101165019B
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propylene
bed reactor
reaction
fluidized
catalyst
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CN101165019A (en
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谢在库
刘俊涛
钟思青
张惠明
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China Petroleum and Chemical Corp
Sinopec Shanghai Research Institute of Petrochemical Technology
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China Petroleum and Chemical Corp
Sinopec Shanghai Research Institute of Petrochemical Technology
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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
    • 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
    • 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
    • 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

Abstract

The present invention relates to one kind of ethylene and propylene producing process with high selectivity and high yield. The production process includes the following steps: 1. reaction of oxygen compound material in the first fluidized bed reactor through contacting with catalyst I to produce effluent I containing ethylene, propylene and C4 and C4+ hydrocarbons; and treating the effluent I ina 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 capable of producing carbon deposit in the second fluidized bed reactor; and 4. returning the deactivated catalyst IVto the first fluidized bed reactor. The production process may be applied in industrial production.

Description

Produce the method for ethene, propylene
Technical field
The present invention relates to a kind of method of producing ethene, propylene, particularly, realize the method for oxygenatedchemicals such as methyl alcohol or dimethyl ether catalysis High-efficient Production ethene, propylene about adopting a regenerated catalyst Passivation Treatment system that regenerated catalyst is carried out Passivation Treatment.
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 production ethene, the method for 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, a kind of method of producing ethene, propylene, may further comprise the steps: (a) be raw material with the oxygenatedchemicals, raw material at first enters with the generation of catalyst I contact reacts from first fluidized bed reactor bottom and contains ethene, propylene, C 4And the effluent I of above hydrocarbon, effluent I discharges from first class bed bioreactor top and enters 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, oxygenatedchemicals is selected from and contains at least a in methyl alcohol or the dme; Passivator is selected from C 1～C 5Alcohol, C 2～C 10Ether, C 4At least a in the above hydro carbons; Catalyst I is selected from least a or its composite molecular screen in aluminium silicophosphate molecular sieve or the ZSM type 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; The temperature of reaction of second fluidized-bed reactor is 100～550 ℃, and reaction pressure is 0.01～1.0MPa, and be 0.1～10 second duration of contact.The temperature of reaction preferable range of first class bed bioreactor 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 passivator preferred version is selected from methyl alcohol, dme, C 4And above hydro carbons at least a.The catalyzer preferred version is selected from least a or its composite molecular screen in SAPO-34 molecular sieve or the ZSM-5 molecular sieve.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; Based on above analysis, the method of production ethene of the present invention, 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.
Adopting technical scheme of the present invention, is catalyzer with the SAPO-34 molecular sieve, and methyl alcohol or dme are raw material, 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 75%, feed stock conversion can reach 100%, has obtained better technical effect.
Description of drawings
Fig. 1 produces the device synoptic diagram of ethene, propylene for oxygenatedchemicals of 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.
Oxygen-containing compound material enters fluidized-bed reactor I1 haptoreaction by inlet device 7 among Fig. 1 from the bottom, and 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.
The invention will be further elaborated below by embodiment, but be not limited only to present embodiment.
Embodiment
[embodiment 1]
Accompanying drawing 1 shown device is adopted in test, is catalyzer with SAPO-34, and methyl alcohol is raw material, and butene-2 is a passivator, and first fluidized bed reactor reaction condition is: 480 ℃ of temperature of reaction, and reaction pressure 0.04MPa, 6 seconds duration of contact, catalyzer and methyl alcohol weight ratio are 1.The second fluidized-bed reactor reaction conditions is: 400 ℃ of temperature of reaction, and pressure 0.06MPa, controlling the second fluid bed reactor catalysis agent carbon deposition quantity is 3%, its reaction result is: yield of ethene 48%, propene yield 31%.
[embodiment 2]
Accompanying drawing 1 shown device is adopted in test, is catalyzer with SAPO-34, and methyl alcohol is raw material, and methyl alcohol is passivator, and first fluidized bed reactor reaction condition is: 450 ℃ of temperature of reaction, and reaction pressure 0.02MPa, 3 seconds duration of contact, catalyzer and methyl alcohol weight ratio are 0.6.The second fluidized-bed reactor reaction conditions is: 470 ℃ of temperature of reaction, and pressure 0.02MPa, controlling the second fluid bed reactor catalysis agent carbon deposition quantity is 2%, its reaction result is: yield of ethene 45%, propene yield 29%.
[embodiment 3]
Accompanying drawing 1 shown device is adopted in test, is catalyzer with SAPO-34, and dme is a raw material, petroleum naphtha is a passivator, and first fluidized bed reactor reaction condition is: 580 ℃ of temperature of reaction, reaction pressure 0.8MPa, 10 seconds duration of contact, catalyzer and dme weight ratio are 1.1.The second fluidized-bed reactor reaction conditions is: 600 ℃ of temperature of reaction, and pressure 0.9MPa, controlling the second fluid bed reactor catalysis agent carbon deposition quantity is 10%, its reaction result is: yield of ethene 42%, propene yield 22%.
[embodiment 4]
Accompanying drawing 1 shown device is adopted in test, with SAPO-34 is catalyzer, dme is a raw material, each hydrocarbon mixture of 50% of C 4 olefin and carbon pentaene hydrocarbon is a passivator, first fluidized bed reactor reaction condition is: 520 ℃ of temperature of reaction, reaction pressure 1.2MPa, 13 seconds duration of contact, catalyzer and dme weight ratio are 6.The second fluidized-bed reactor reaction conditions is: 500 ℃ of temperature of reaction, and pressure 1.5MPa, controlling the second fluid bed reactor catalysis agent carbon deposition quantity is 4%, its reaction result is: yield of ethene 44%, propene yield 28%.
[embodiment 5]
Accompanying drawing 1 shown device is adopted in test, with SAPO-34 is catalyzer, methyl alcohol and dme are raw material, wherein the weight ratio of methyl alcohol and dme is 1: 2, the trimethyl carbinol is a passivator, and first fluidized bed reactor reaction condition is: 540 ℃ of temperature of reaction, reaction pressure 0.2MPa, 4 seconds duration of contact, catalyzer is 0.5 with the raw material weight ratio.The second fluidized-bed reactor reaction conditions is: 530 ℃ of temperature of reaction, and pressure 0.3MPa, controlling the second fluid bed reactor catalysis agent carbon deposition quantity is 7%, its reaction result is: yield of ethene 48%, propene yield 30%.
[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, and SAPO-34 accounts for 80%, and methyl alcohol and dme are raw material, wherein the weight ratio of methyl alcohol and dme is 2: 1, methyl tertiary butyl ether is a passivator, and 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 30%, propene yield 38%.
[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, and SAPO-34 accounts for 80%, and methyl alcohol and dme are raw material, wherein the weight ratio of methyl alcohol and dme is 3: 1, hexichol, toluene and ethyl benzene mixtures are passivator, and first fluidized bed reactor reaction condition is: 530 ℃ of temperature of reaction, reaction pressure 0.4MPa, 4 seconds duration of contact, catalyzer is 0.7 with the raw material weight ratio.The second fluidized-bed reactor reaction conditions is: 580 ℃ of temperature of reaction, and pressure 0.5MPa, controlling the second fluid bed reactor catalysis agent carbon deposition quantity is 7%, its reaction result is: yield of ethene 35%, propene yield 31%.
[embodiment 8]
Accompanying drawing 1 shown device is adopted in test, and according to condition and the catalyzer of embodiment 7, just catalyzer adopts the ZSM-5 molecular sieve, and in its reaction product, yield of ethene is 12%, and propene yield is 48%.
[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 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 43%, and propene yield is 27%.

Claims (6)

1. method of producing ethene and propylene may further comprise the steps:
(a) with the oxygenatedchemicals be raw material, raw material at first enters with the generation of catalyst I contact reacts from first fluidized bed reactor bottom and contains ethene, propylene, C 4And the effluent I of above hydrocarbon, effluent I discharges from first class bed bioreactor top and enters 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, oxygenatedchemicals is selected from and contains at least a in methyl alcohol or the dme; Passivator is selected from C 1～C 5Alcohol, C 2～C 10At least a in ether or the petroleum naphtha; Catalyst I is selected from least a or its composite molecular screen in aluminium silicophosphate molecular sieve or the ZSM type molecular sieve.
2. according to the method for described production 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; The temperature of reaction of second fluidized-bed reactor is 100～550 ℃, and reaction pressure is 0.01～1.0MPa, and be 0.1～10 second duration of contact.
3. according to the method for described production ethene of claim 2 and propylene, the temperature of reaction that it is characterized in that the first class bed bioreactor 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 method for described production ethene of claim 1 and propylene, it is characterized in that passivator is selected from least a in methyl alcohol, dme or the petroleum naphtha.
5. according to the method for described production ethene of claim 1 and propylene, it is characterized in that described catalyzer is selected from SAPO-34 molecular sieve or ZSM-5 molecular sieve.
6. according to the method for described production 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.
CN2006101173450A 2006-10-20 2006-10-20 Method for producing ethylene and propylene Active CN101165019B (en)

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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
EA024895B1 (en) * 2011-12-19 2016-10-31 Далянь Инститьют Оф Кемикал Физикс, Чайниз Академи Оф Сайенсез Catalyst for preparing ethylene and propylene from methanol and/or dimethyl ether, preparation and use thereof
CN111889037B (en) * 2020-08-06 2023-02-28 中国石油化工股份有限公司 Moving bed reactor and reaction method suitable for heat coupling or reaction coupling
CN111974462A (en) * 2020-09-01 2020-11-24 大唐国际化工技术研究院有限公司 Method for recycling waste MTP catalyst
CN116375551B (en) * 2023-04-14 2024-03-29 浙江大学 Method for preparing ethylene from alkoxy benzene with high selectivity

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