CN104557366B - System and method for preparing ethylene, propylene and aromatic hydrocarbon by converting methanol and/or dimethyl ether - Google Patents
System and method for preparing ethylene, propylene and aromatic hydrocarbon by converting methanol and/or dimethyl ether Download PDFInfo
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- CN104557366B CN104557366B CN201310512501.3A CN201310512501A CN104557366B CN 104557366 B CN104557366 B CN 104557366B CN 201310512501 A CN201310512501 A CN 201310512501A CN 104557366 B CN104557366 B CN 104557366B
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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
Abstract
The invention relates to a system and method for preparing ethylene, propylene and aromatic hydrocarbon by converting methanol and/or dimethyl ether and mainly aims to solve the problem of low yield of ethylene, propylene and aromatic hydrocarbon in the prior art. The system comprises a reactor I (1), a reactor II (2), a regenerator (3) and a stripper (4). Methanol and/or dimethyl ether (7) and a recyclable material (8) are respectively subjected to contact reaction with a catalyst I in the reactor I (1) and the reactor II (2), a carbon deposited catalyst II after reaction is added into the stripper (4), a carbon deposited catalyst III after stripping is added into the regenerator (3) through an inclined regeneration tube (13) and is regenerated, and a catalyst I after regeneration is added into the reactor I (1) and the reactor II (2) through an inclined regeneration tube I (5) and an inclined regeneration tube II (6). By adopting the technical scheme, the problem of low yield of ethylene, propylene and aromatic hydrocarbon can be well solved. The system and the method can be applied to the industrial production of ethylene, propylene and aromatic hydrocarbon.
Description
Technical field
The present invention relates to the system and method for a kind of methyl alcohol and/or dimethyl ether conversion ethene, propylene and aromatic hydrocarbons.
Background technology
Ethene, propylene and aromatic hydrocarbons (especially triphen, benzene benzene, toluene toluene, dimethylbenzene xylene, i.e. btx)
It is important basic organic synthesis raw material.Driven by downstream derivative thing demand, the market demand of ethene, propylene and aromatic hydrocarbons continues
Increase.
It is ethene, propylene and virtue with liquid hydrocarbon (as naphtha, the diesel oil, secondary operation oil) steam cracking process as raw material
The main production of hydrocarbon.This technique belongs to petroleum path production technology, in recent years, due to the limited supply of petroleum resources and
Higher price, cost of material is continuously increased.By factor, alternative materials prepare ethene, propylene and aromatic hydrocarbons technology cause more next
More widely pay close attention to.Wherein, for coal-based methanol, dimethyl ether raw material, due to rich coal resources in China, it is increasingly becoming one kind
Important Chemical Manufacture raw material, becomes the important supplement of petroleum.Accordingly, it is considered to methyl alcohol and/or dimethyl ether for raw material system
Standby ethene, propylene and aromatic hydrocarbons.
In various existing methyl alcohol, dimethyl ether catalysis transformation technology, the product of methanol/dimethyl ether conversion aromatic hydrocarbons is simultaneously
Including ethene, propylene and aromatic hydrocarbons.This technology initially sees chang of mobil company in 1977 et al. (journal of
Catalysis, 1977,47,249) report methyl alcohol and its oxygenatedchemicals conversion preparation virtue on zsm-5 molecular sieve catalyst
The method of the hydrocarbons such as hydrocarbon.1985, in United States Patent (USP) us1590321 that mobil company applies at it, disclose first
Methyl alcohol, the result of study of dimethyl ether conversion aromatic hydrocarbons, this research is using the phosphorous zsm-5 molecular sieve being 2.7 weight % for being catalyzed
Agent, reaction temperature is 400 ~ 450 DEG C, methyl alcohol, dimethyl ether air speed 1.3 (Grams Per Hour)/gram catalyst.
The relevant report in this field and patent are more, but the purpose product of most of technology is aromatic hydrocarbons, and ethene, propylene belong to
In accessory substance, yield is low.Such as, the patent in terms of methyl alcohol arenes catalytic agent: Chinese patent cn102372535,
cn102371176、cn102371177、cn102372550、cn102372536、cn102371178、cn102416342、
Cn101550051, United States Patent (USP) us4615995, us2002/0099249a1 etc..Such as, in terms of methyl alcohol aromatics process
Patent: United States Patent (USP) us4686312, Chinese patent zl101244969, zl1880288, cn101602646,
Cn101823929, cn101671226, cn102199069, cn102199446, cn1880288 etc..
In addition, technology path disclosed in some patents be while methyl alcohol aromatic hydrocarbons co-producing light olefins, gasoline etc. other
Product, such as patent cn102775261, cn102146010, cn102531821, cn102190546, cn102372537 etc..
Wherein, Multi-function methanol processing method disclosed in patent cn102775261 and device utilize methanol production low-carbon (LC) alkene
Hydrocarbon, gasoline, aromatic hydrocarbons.The method adopts two-step method production technology, and first step methanol feedstock produces low under special-purpose catalyst 1 effect
Carbon olefin, second step by the reaction gas containing low-carbon alkene after heat exchange, chilling, carrying out washing treatment, in the presence of special-purpose catalyst 2
Synthesis aromatic hydrocarbons and/or gasoline.The reactor of two courses of reaction can be fixed bed or fluid bed.The method adopts two-step method, technique
Flow process is complicated.
Patent cn102146010 discloses the work producing low-carbon alkene and arene parallel cogeneration gasoline with methyl alcohol for raw material
Skill.Low-carbon alkene and aromatic hydrocarbons are produced for raw material and using molecular sieve catalyst through methyl alcohol alkylation reaction and aromatization with methyl alcohol
Co-production gasoline.The reactor of methyl alcohol alkylation reaction and aromatization is various types of fixed bed reactors, pressure 0.01 ~
0.5 MPa, 180 ~ 600 DEG C of temperature.Total liquid yield is more than 70 weight %, and triphen yield is more than 90 weight %.The method is also adopted by two
Reactor, technological process is complicated.
Patent cn102531821 discloses methyl alcohol and the co-fed method producing low-carbon alkene and/or aromatic hydrocarbons of naphtha,
Using the zsm-5 catalyst of load 2.2 ~ 6.0 weight %la and 1.0 ~ 2.8 weight %p, fixed bed reactors or fluid bed can be adopted
Reactor.Reaction temperature is 550 ~ 670 DEG C, air speed 1.0 ~ 5 (Grams Per Hour)/gram catalyst.The triolefin yield of the method is higher,
But btx yield is low, only 5 ~ 17 weight %.
The method that patent cn102372537 and cn102190546 disclose preparing propylene by methanol transformation and aromatic hydrocarbons.This two specially
Profit is to develop on the basis of preparing propylene by methanol transformation technology, and propylene is main purpose product, and aromatics yield is relatively low.
All there is a problem of in above-mentioned patented technology that ethene, propylene and aromatics yield are low.The present invention pointedly proposes
Technical scheme, solves the problems referred to above.
Content of the invention
One of problem to be solved by this invention is ethene in prior art, propylene and the low technical problem of aromatics yield,
A kind of methyl alcohol and/or the system of dimethyl ether conversion ethene, propylene and aromatic hydrocarbons are provided.This system has ethene, propylene and aromatic hydrocarbons
The advantage of high income.
The two of the technical problem to be solved are to provide a kind of method corresponding with solving one of technical problem.
For one of solving the above problems, the technical solution used in the present invention is as follows: a kind of methyl alcohol and/or dimethyl ether conversion system
The system of ethene, propylene and aromatic hydrocarbons, including reactor 1, reactor 2, regenerator 3, stripper 4, methyl alcohol and/or dimethyl ether
7th, respectively in reactor 1, reactor 2 catalyst neutralisation haptoreaction, reacted carbon deposited catalyst enters recycle stock 8
Enter stripper 4, the carbon deposited catalyst after stripping enters regenerator 3 through regenerator sloped tube 13 and regenerates, and the catalyst after regeneration is through again
Raw inclined tube 5, regenerator sloped tube 6 respectively enter reactor 1, reactor 2.
In technique scheme, methyl alcohol and/or dimethyl ether are converted into catalyst haptoreaction with second in reactor 1
Product based on alkene, propylene and aromatic hydrocarbons；Recycle stock reactor 2 catalyst neutralisation haptoreaction be converted into ethene, third
Product based on alkene and aromatic hydrocarbons；Carbon deposited catalyst is stripped off the product carrying in stripper 4；Carbon deposited catalyst exists
Regenerator 3 removes coke by way of burning.
In technique scheme, reactor 1, for being converted into methyl alcohol and/or dimethyl ether and catalyst haptoreaction
Product based on ethene, propylene and aromatic hydrocarbons；Reactor 2, for by recycle stock and catalyst haptoreaction be converted into
Product based on ethene, propylene and aromatic hydrocarbons；Regenerator 3, for removing the coke on carbon deposited catalyst by way of burning；
Stripper 4, for being stripped off the product carrying on carbon deposited catalyst.
For solve the above problems two, the technical solution used in the present invention is as follows: a kind of methyl alcohol and/or dimethyl ether conversion system
The method of ethene, propylene and aromatic hydrocarbons, using said system, described method includes following step:
A) methyl alcohol and/or dimethyl ether 7 in reactor 1 with catalyst haptoreaction, recycle stock 8 is in reactor 2
Catalyst neutralisation haptoreaction, reaction of formation product and carbon deposited catalyst enter stripper 4 and contact with stripping fluid 10, obtain
To product 9 and carbon deposited catalyst；
B) carbon deposited catalyst enters regenerator 3 through regenerator sloped tube 13；
C) carbon deposited catalyst contacts with regenerating medium 11 in regenerator 3 and burns, and obtains catalyst and flue gas 12；
D) catalyst respectively enters reactor 1, reactor 2 through regenerator sloped tube 5, regenerator sloped tube 6；
E) product 9 enters subsequent separation system, and part ethane, propane, the non-aromatic conduct of c4 and c5 and c6 in product follows
Ring material 8 proceeds to react, and remaining product using ethene, propylene, BTX aromatics based on is as output of products system.
In technique scheme, the reaction temperature of reactor 1 is 400 ~ 550 DEG C, counts reaction pressure for 0 ~ 0.5 with gauge pressure
MPa, weight space velocity is 2 ~ 10 (Grams Per Hours)/gram catalyst, the matter of catalyst internal circulating load and methyl alcohol and/or dimethyl ether inlet amount
Amount ratio is for 3～30: 1, catalyst in reactor density is 50～150 kgs/m3, average gas superficial velocity 0.7 ~ 4 meter per second.?
Under a large amount of ethene, propylene operator scheme, reaction temperature is 480 ~ 550 DEG C, counts reaction pressure for 0 ~ 0.3 MPa with gauge pressure, weight
Air speed is 4 ~ 10 (Grams Per Hours)/gram catalyst, and the mass ratio of catalyst internal circulating load and methyl alcohol and/or dimethyl ether inlet amount is 10
～30: 1, catalyst in reactor density is 50～120 kgs/m3, average gas superficial velocity 1.3 ~ 4 meter per second；Maximum aromatic hydrocarbons
Under operator scheme, reaction temperature is 400 ~ 500 DEG C, counts reaction pressure for 0.1 ~ 0.5 MPa with gauge pressure, and weight space velocity is 2 ~ 4
(Grams Per Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and methyl alcohol and/or dimethyl ether inlet amount is 3～25: 1, reaction
In device, density of catalyst is 80～150 kgs/m3, average gas superficial velocity 0.7 ~ 1.3 meter per second；Coproduction ethene, propylene and aromatic hydrocarbons
Under pattern, reaction temperature is 440 ~ 520 DEG C, counts reaction pressure for 0.1 ~ 0.4 MPa with gauge pressure, weight space velocity for 2 ~ 7 (gram/little
When)/gram catalyst, the mass ratio of catalyst internal circulating load and methyl alcohol and/or dimethyl ether inlet amount is 5～25: 1, urges in reactor
Agent density is 70～130 kgs/m3, average gas superficial velocity 0.7 ~ 2.3 meter per second.
In technique scheme, the reaction temperature of reactor 2 is 430 ~ 650 DEG C, counts reaction pressure for 0 ~ 0.5 with gauge pressure
MPa, weight space velocity is 2 ~ 20 (Grams Per Hours)/gram catalyst, catalyst internal circulating load and methyl alcohol and/or dimethyl ether inlet amount
Mass ratio is 5～40: 1, and catalyst in reactor density is 50～150 kgs/m3, average gas superficial velocity 0.7 ~ 7 meter per second.
Under maximum ethene, propylene operator scheme, reaction temperature is 550 ~ 650 DEG C, counts reaction pressure for 0 ~ 0.3 MPa with gauge pressure, weight
Amount air speed is 6 ~ 20 (Grams Per Hours)/gram catalyst, and the mass ratio of catalyst internal circulating load and methyl alcohol and/or dimethyl ether inlet amount is
10～40: 1, catalyst in reactor density is 50～120 kgs/m3, average gas superficial velocity 2 ~ 7 meter per second；Maximum virtue
Under hydrocarbon operator scheme, reaction temperature is 430 ~ 520 DEG C, counts reaction pressure for 0.1 ~ 0.5 MPa with gauge pressure, and weight space velocity is 2 ~ 6
(Grams Per Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and methyl alcohol and/or dimethyl ether inlet amount is 5～25: 1, reaction
In device, density of catalyst is 80～150 kgs/m3, average gas superficial velocity 0.7 ~ 2 meter per second；Coproduction ethene, propylene and aromatic hydrocarbons mould
Under formula, reaction temperature is 440 ~ 520 DEG C, counts reaction pressure for 0.1 ~ 0.4 MPa with gauge pressure, weight space velocity for 2 ~ 15 (gram/little
When)/gram catalyst, the mass ratio of catalyst internal circulating load and methyl alcohol and/or dimethyl ether inlet amount is 8～35: 1, urges in reactor
Agent density is 70～130 kgs/m3, average gas superficial velocity 0.7 ~ 4.8 meter per second.
In technique scheme, catalyst activity component is that zsm-5, zsm-23, zsm-11, β, y or mutual are formed
Composite molecular screen, preferably zsm-5；Carrier is kaolin, aluminum oxide, silica；The mass ratio of active component and carrier is (10
~ 50): (50 ~ 90), preferably (20 ~ 40): (60 ~ 80).
In technique scheme, catalyst is loaded with one or more element or oxidation in zn, ag, p, ga, cu, mn, mg
Thing, preferably zn, p；With the mass percent of catalyst, the element of load content on a catalyst is 0.01 ~ 15 weight %,
Preferably 0.02 ~ 8 weight %.
In technique scheme, the active component of catalyst is selected from zsm-5 molecular sieve, with the percentage by weight of catalyst
Meter, catalyst loads zn element or oxide, the p element of 0.1 ~ 8 weight % or the oxide of 0.01 ~ 5 weight %.
In technique scheme, raw material can be methyl alcohol or dimethyl ether or both mixtures.
In technique scheme, in raw material, the weight/mass percentage composition of water is 0 ~ 30 weight %, preferably shorter than 10 weight %.
In technique scheme, stripping fluid 10 is water vapour, n2Or both mixtures, regenerating medium 11 be air,
o2、n2Or the mixture of both or three.
In technique scheme, the percentage composition that the coke on catalyst accounts for catalyst gross mass is less than 0.1 weight %.
The present invention circulates profit by the separation of product during methyl alcohol and/or dimethyl ether catalysis conversion reaction and accessory substance
With realizing improving the purpose of the yield of ethene, propylene and aromatic hydrocarbons.
The technical scheme that the present invention provides, methyl alcohol and/or dimethyl ether and accessory substance are carried out instead respectively in two reactors
Should, different reaction conditions may be selected, realize different production purposes respectively, be mutually combined, such that it is able to conveniently realize
A large amount of ethene, propylene, maximum aromatic hydrocarbons and coproduction ethene, propylene and three kinds of operator schemes of aromatic hydrocarbons.
Using technical scheme, operate under maximum ethene, propylene pattern, the reaction temperature of reactor is
500 DEG C, reaction pressure is counted for 0.2 MPa with gauge pressure, weight space velocity be 5 (Grams Per Hours)/gram catalyst, catalyst internal circulating load and
The mass ratio of methyl alcohol and/or dimethyl ether inlet amount is 15: 1, and catalyst in reactor density is 70 kgs/m3, average void tower
Gas speed 1.6 meter per seconds；The reaction temperature of reactor is 580 DEG C, counts reaction pressure for 0.2 MPa with gauge pressure, and weight space velocity is 8
(Grams Per Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and methyl alcohol and/or dimethyl ether inlet amount is 20: 1, in reactor
Density of catalyst is 60 kgs/m3, average gas superficial velocity 2.7 meter per second；Using cu-zsm-5 catalyst；Methyl alcohol feeds；Ethene
Carbon base absorption rate is 28.3 weight %, propylene carbon base absorption rate is 25.4 weight %, aromatic hydrocarbons carbon base absorption rate is 34.9 weight %.
Using technical scheme, operate under maximum aromatic hydrocarbons pattern, the reaction temperature of reactor is 475 DEG C,
Reaction pressure is counted for 0.25 MPa with gauge pressure, weight space velocity is 2 (Grams Per Hours)/gram catalyst, catalyst internal circulating load and methyl alcohol
And/or the mass ratio of dimethyl ether inlet amount is 7: 1, catalyst in reactor density is 140 kgs/m3, average gas superficial velocity
0.7 meter per second；The reaction temperature of reactor is 480 DEG C, counts reaction pressure for 0.25 MPa with gauge pressure, and weight space velocity is 2
(Grams Per Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and methyl alcohol and/or dimethyl ether inlet amount is 10: 1, in reactor
Density of catalyst is 130 kgs/m3, average gas superficial velocity 0.7 meter per second；Using zn-p-zsm-5 catalyst；Methyl alcohol feeds；
Ethene carbon base absorption rate is 14.1 weight %, propylene carbon base absorption rate is 11.5 weight %, aromatic hydrocarbons carbon base absorption rate is 66.4 weight %, btx carbon
Base yield is 47.8 weight %.
Using technical scheme, operate under coproduction ethene, propylene and aromatic hydrocarbons pattern, the reaction temperature of reactor
Spend for 460 DEG C, reaction pressure is counted for 0.2 MPa with gauge pressure, weight space velocity is 3 (Grams Per Hours)/gram catalyst, catalyst circulates
The mass ratio of amount and methyl alcohol and/or dimethyl ether inlet amount is 12: 1, and catalyst in reactor density is 120 kgs/m3, averagely
Empty tower gas velocity 1 meter per second；The reaction temperature of reactor is 520 DEG C, counts reaction pressure for 0.2 MPa with gauge pressure, weight space velocity is
4 (Grams Per Hours)/gram catalyst, the mass ratio of catalyst internal circulating load and methyl alcohol and/or dimethyl ether inlet amount is 14: 1, reactor
Interior density of catalyst is double centner/rice3, average gas superficial velocity 1.3 meter per second；Using zn-mg-p-zsm-5 catalyst；Methyl alcohol enters
Material；Ethene carbon base absorption rate is 20.4 weight %, propylene carbon base absorption rate is 18.7 weight %, aromatic hydrocarbons carbon base absorption rate is 48.3 weight %,
Btx carbon base absorption rate is 34.8 weight %.
Brief description
Fig. 1, Fig. 2 are the schematic device of technical scheme of the present invention.
In Fig. 1 ~ 2,1 is reactor；2 is reactor；3 is regenerator；4 is stripper；5 is oblique for the regeneration of reactor
Pipe；6 is the regenerator sloped tube of reactor；7 is methyl alcohol and/or dimethyl ether；8 is recycle stock；9 is product；10 is stripping
Medium；11 is regenerating medium；12 is flue gas；13 is inclined tube to be generated.
In Fig. 1 methyl alcohol and/or dimethyl ether 7 in reactor 1 with catalyst haptoreaction, recycle stock 8 is in reactor
2 catalyst neutralisation haptoreactions, reaction of formation product and carbon deposited catalyst enter stripper 4 and contact with stripping fluid 10,
Obtain product 9 and carbon deposited catalyst；Carbon deposited catalyst enters regenerator 3 through regenerator sloped tube 13；Carbon deposited catalyst
Regenerator 3 contacts with regenerating medium 11 and burns, obtain catalyst and flue gas 12；Product 9 enters later separation system
System, part ethane in product, propane, c4 and c5 and c6 are non-aromatic to be proceeded to react as recycle stock 8, remaining with ethene, third
Product based on alkene, BTX aromatics is as output of products system.
In Fig. 2 methyl alcohol and/or dimethyl ether 7 in reactor 1 with catalyst haptoreaction, recycle stock 8 is in reactor
2 catalyst neutralisation haptoreactions, reaction of formation product and carbon deposited catalyst enter stripper 4 and contact with stripping fluid 10,
Obtain product 9 and carbon deposited catalyst；Carbon deposited catalyst enters regenerator 3；Carbon deposited catalyst neutralizes in regenerator 3
Regenerating medium 11 contact is burnt, and obtains catalyst and flue gas 12；Product 9 enters subsequent separation system, part second in product
Alkane, propane, c4 and c5 and c6 are non-aromatic to be proceeded to react as recycle stock 8, and remaining is based on ethene, propylene, BTX aromatics
Product as output of products system.
Specific embodiment
[embodiment 1]
Using device as shown in Figure 1.
The reaction condition of reactor is: 500 DEG C of temperature, 0.2 MPa of reaction pressure in terms of gauge pressure, weight space velocity 5 (gram/
Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and feedstock amount is 15: 1, and catalyst in reactor density is 70
Kg/m3, average gas superficial velocity 1.6 meter per second.With methyl alcohol as raw material, water content is 5 weight %.
The reaction condition of reactor is: 580 DEG C of temperature, 0.2 MPa of reaction pressure in terms of gauge pressure, weight space velocity 8 (gram/
Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and feedstock amount is 20: 1, and catalyst in reactor density is 60
Kg/m3, average gas superficial velocity 2.7 meter per second.In raw material, the non-aromatic mass ratio of ethane propane c4 and c5 and c6 is 2:3:5.
Using cu-zsm-5 catalyst.
The preparation process of cu-zsm-5 catalyst: zsm-5 molecular sieve, carrier and binding agent mechanical mixture add appropriate
Water, hcl, control ph value not less than 3, and slurries stir spray shaping at 500 DEG C, and the zsm-5 making 60 ~ 300 mesh urges
Agent intermediate.The mass ratio of zsm-5 molecular sieve and matrix is 4:6；The silicoaluminophosphate molecular of zsm-5 molecular sieve is than for 25；Matrix is
Kaolin and the mixture of alundum (Al2O3), both mass ratioes are 7:3.The solution that cu mass of ion percentage composition is 5%,
Impregnated than for 1.74:1 with the weight of solution and catalyst, be dried 5 hours at 120 DEG C, place into Muffle furnace in 550 DEG C
Lower roasting is prepared into the cu-zsm-5 catalyst that cu constituent content is 8 weight % for 6 hours.
[embodiment 2]
Using device as shown in Figure 1.
The reaction condition of reactor is: 400 DEG C of temperature, 0.5 MPa of reaction pressure in terms of gauge pressure, weight space velocity 10 (gram/
Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and feedstock amount is 3: 1, and catalyst in reactor density is 50,000
Grams m3, average gas superficial velocity 0.7 meter per second.With methyl alcohol as raw material.
The reaction condition of reactor is: 430 DEG C of temperature, 0.5 MPa of reaction pressure in terms of gauge pressure, weight space velocity 20
(Grams Per Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and feedstock amount is 5: 1, and catalyst in reactor density is
50 kgs/m3, average gas superficial velocity 2 meter per second.In raw material, the non-aromatic mass ratio of ethane propane c4 and c5 and c6 is 1:1:8.
Using ag-y-zsm-23 catalyst.
The preparation process of ag-y-zsm-23 catalyst: will be mixed to y molecular sieve, zsm-23 molecular sieve, carrier and binding agent machinery
Close, add suitable quantity of water, hcl, control ph value not less than 3, slurries stir spray shaping at 500 DEG C, make 60 ~ 300
Purpose y-zsm-23 catalyst intermediate.The mass ratio of molecular sieve and matrix is 1:9；Y molecular sieve and zsm-23 molecular sieve quality
Than for 3:7；The silicoaluminophosphate molecular of y molecular sieve is than for 10；The silicoaluminophosphate molecular of zsm-23 molecular sieve is than for 60；Matrix is kaolin and three
The mixture of Al 2 O, both mass ratioes are 8:2.The solution that ag mass of ion percentage composition is 1%, with solution and urging
Agent weight is impregnated than for 0.1:1, is dried 5 hours at 120 DEG C, places into Muffle furnace 6 hours systems of roasting at 550 DEG C
Standby one-tenth ag constituent content is the ag-y-zsm-23 catalyst of 0.1 weight %.
[embodiment 3]
Using device as shown in Figure 1.
The reaction condition of reactor is: 550 DEG C of temperature, 0 MPa of reaction pressure in terms of gauge pressure, weight space velocity 10 (gram/little
When)/gram catalyst.With methyl alcohol as raw material, the mass ratio of catalyst internal circulating load and feedstock amount is catalysis in 30: 1, reactor
Agent density is 150 kgs/m3, average gas superficial velocity 4 meter per second.
The reaction condition of reactor is: 650 DEG C of temperature, 0 MPa of reaction pressure in terms of gauge pressure, weight space velocity 20 (gram/
Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and feedstock amount is 40: 1, and catalyst in reactor density is 150
Kg/m3, average gas superficial velocity 7 meter per second.In raw material, the non-aromatic mass ratio of propane c4 and c5 and c6 is 2:8.
Using ga- beta catalyst.
The preparation process of ga- beta catalyst: beta-molecular sieve, carrier and binding agent mechanical mixture add suitable quantity of water, hcl, control
Ph value processed is not less than 4, and slurries stir spray shaping at 500 DEG C, make the beta catalyst intermediate of 60 ~ 300 mesh.β divides
The mass ratio of son sieve and matrix is 5:5；The silicoaluminophosphate molecular of beta-molecular sieve is than for 20；Matrix is that kaolin, silica and three aoxidize
The mixture of two aluminium, the mass ratio of three is 7:1:2.The solution that ga mass of ion percentage composition is 2%, with solution and catalysis
Agent weight is impregnated than for 0.4:1, is dried 5 hours at 120 DEG C, places into Muffle furnace roasting preparation in 6 hours at 550 DEG C
Become the ga- beta catalyst that ga constituent content is 0.8 weight %.
[embodiment 4]
Using device as shown in Figure 1.
The reaction condition of reactor is: 480 DEG C of temperature, 0.3 MPa of reaction pressure in terms of gauge pressure, weight space velocity 3 (gram/
Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and feedstock amount is 9: 1, and catalyst in reactor density is 110
Kg/m3, average gas superficial velocity 1.1 meter per second.With dimethyl ether as raw material.
The reaction condition of reactor is: 530 DEG C of temperature, 0.3 MPa of reaction pressure in terms of gauge pressure, weight space velocity 7 (gram/
Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and feedstock amount is 15: 1, and catalyst in reactor density is 80
Kg/m3, average gas superficial velocity 2.2 meter per second.In raw material, the non-aromatic mass ratio of ethane c4 and c5 and c6 is 3:7.
Using mn-zsm-11 catalyst.
The preparation process of mn-zsm-11 catalyst: zsm-11 molecular sieve, carrier and binding agent mechanical mixture add suitable
Amount water, hcl, control ph value not less than 3, and slurries stir spray shaping at 500 DEG C, make the zsm-11 of 60 ~ 300 mesh
Catalyst intermediate.The mass ratio of zsm-11 molecular sieve and matrix is 3:7；The silicoaluminophosphate molecular of zsm-11 molecular sieve is than for 50；Base
Matter is the mixture of kaolin and alundum (Al2O3), and both mass ratioes are 7:3.Mn mass of ion percentage composition is 10%
Solution, is impregnated with the weight of solution and catalyst than for 1:1, is dried 5 hours at 120 DEG C, places into Muffle furnace in 550
At DEG C, roasting is prepared into the mn-zsm-11 catalyst that mn constituent content is 9.09 weight % for 6 hours.
[embodiment 5]
Using device as shown in Figure 1.
The reaction condition of reactor is: 475 DEG C of temperature, 0.25 MPa of reaction pressure in terms of gauge pressure, weight space velocity 2 (gram/
Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and feedstock amount is 7: 1, and catalyst in reactor density is 140
Kg/m3, average gas superficial velocity 0.7 meter per second.With methyl alcohol as raw material.
The reaction condition of reactor is: 480 DEG C of temperature, 0.25 MPa of reaction pressure in terms of gauge pressure, weight space velocity 2 (gram/
Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and feedstock amount is 10: 1, and catalyst in reactor density is 130
Kg/m3, average gas superficial velocity 0.7 meter per second.In raw material, the mass ratio of ethane propane is 5:5.
Using zn-p-zsm-5 catalyst.
The preparation process of zn-p-zsm-5 catalyst: zsm-5 molecular sieve, carrier and binding agent mechanical mixture add suitable
Amount water, h3po4, control ph value not less than 3, slurries stir spray shaping at 500 DEG C, make the p- of 60 ~ 300 mesh
Zsm-5 catalyst intermediate.h3po4The concentration of solution is 1 weight %, and the weight of solution and molecular sieve ratio is for 1.53:1.Zsm-5 divides
The mass ratio of son sieve and matrix is 3.5:6.5；The silicoaluminophosphate molecular of zsm-5 molecular sieve is than for 25；Matrix is kaolin and three oxidations
The mixture of two aluminium, both mass ratioes are 7:3.The solution that zn mass of ion percentage composition is 5%, with solution and p-zsm-5
Catalyst weight is impregnated than for 0.6:1, is dried 5 hours, places into Muffle furnace roasting 6 at 550 DEG C little at 120 DEG C
When, being prepared into zn constituent content is 2.87 weight %, and p element content is the zn-p-zsm-5 catalyst of 1.48 weight %.
[embodiment 6]
Using device as shown in Figure 2.
The reaction condition of reactor is: 480 DEG C of temperature, 0.1 MPa of reaction pressure in terms of gauge pressure, weight space velocity 4 (gram/
Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and feedstock amount is 10: 1, and catalyst in reactor density is 90
Kg/m3, average gas superficial velocity 1.3 meter per second.With methyl alcohol as raw material.
The reaction condition of reactor is: 580 DEG C of temperature, 0.1 MPa of reaction pressure in terms of gauge pressure, weight space velocity 10
(Grams Per Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and feedstock amount is 30: 1, catalyst in reactor density
For 70 kgs/m3, average gas superficial velocity 3.3 meter per second.In raw material, the non-aromatic mass ratio of ethane propane c4 and c5 and c6 is 3:
3:4.
Using zsm-5- beta catalyst.
The preparation process of zsm-5- beta catalyst: by zsm-5 molecular sieve, beta-molecular sieve, carrier and binding agent mechanical mixture, plus
Enter suitable quantity of water, hcl, control ph value not less than 3, slurries stir spray shaping at 500 DEG C, make 60 ~ 300 purposes
Zsm-5- beta catalyst.The mass ratio of zsm-5 and beta-molecular sieve and matrix is 3.5: 6.5.The silicoaluminophosphate molecular ratio of zsm-5 molecular sieve is
38；The silicoaluminophosphate molecular of beta-molecular sieve is than for 20；The mass ratio of zsm-5 and beta-molecular sieve is 9:1.Matrix is kaolin, silica
With the mixture of alundum (Al2O3), the mass ratio of three is 5:2:3.
[embodiment 7]
Using device as shown in Figure 2.
The reaction condition of reactor is: 450 DEG C of temperature, 0.15 MPa of reaction pressure in terms of gauge pressure, weight space velocity 5 (gram/
Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and feedstock amount is 5: 1, and catalyst in reactor density is 80
Kg/m3, average gas superficial velocity 1.6 meter per second.With methyl alcohol as raw material.
The reaction condition of reactor is: 550 DEG C of temperature, 0.15 MPa of reaction pressure in terms of gauge pressure, weight space velocity 7
(Grams Per Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and feedstock amount is 20: 1, catalyst in reactor density
For 70 kgs/m3, average gas superficial velocity 2.1 meter per second.In raw material, the non-aromatic mass ratio of ethane propane c4 and c5 and c6 is
0.5:0.5:9.
Using zn-ag-p-zsm-5 catalyst.
The preparation process of zn-ag-p-zsm-5 catalyst: zsm-5 molecular sieve, carrier and binding agent mechanical mixture add
Suitable quantity of water, h3po4, control ph value not less than 3, slurries stir spray shaping at 500 DEG C, make the p- of 60 ~ 300 mesh
Zsm-5 catalyst intermediate.h3po4The concentration of solution is 2.5 weight %, and the weight of solution and molecular sieve ratio is for 2:1.Zsm-5 divides
The mass ratio of son sieve and matrix is 3.5:6.5；The silicoaluminophosphate molecular of zsm-5 molecular sieve is than for 28；Matrix is kaolin and three oxidations
The mixture of two aluminium, both mass ratioes are 8:2.Ag mass of ion percentage composition is that 1%, zn mass of ion percentage composition is
3% solution, is impregnated with solution and p-zsm-5 catalyst weight than for 0.8:1, is dried 5 hours, places at 120 DEG C
Muffle furnace roasting 6 hours at 550 DEG C, being prepared into zn constituent content is 2.32 weight %, and ag constituent content is 0.78 weight %, p
Constituent content is the zn-ag-p-zsm-5 catalyst of 1.51 weight %.
[embodiment 8]
Using device as shown in Figure 2.
The reaction condition of reactor is: 460 DEG C of temperature, 0.2 MPa of reaction pressure in terms of gauge pressure, weight space velocity 3 (gram/little
When)/gram catalyst, the mass ratio of catalyst internal circulating load and feedstock amount is 12: 1, and catalyst in reactor density is 120
Kg/m3, average gas superficial velocity 1 meter per second.With methyl alcohol as raw material.
The reaction condition of reactor is: 520 DEG C of temperature, 0.2 MPa of reaction pressure in terms of gauge pressure, weight space velocity 4 (gram/
Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and feedstock amount is 14: 1, and catalyst in reactor density is 100
Kg/m3, average gas superficial velocity 1.3 meter per second.In raw material, the non-aromatic mass ratio of ethane propane c4 and c5 and c6 is 1:1:8.
Using zn-mg-p-zsm-5 catalyst.
The preparation process of zn-mg-p-zsm-5 catalyst: zsm-5 molecular sieve, carrier and binding agent mechanical mixture add
Suitable quantity of water, h3po4, control ph value not less than 3, slurries stir spray shaping at 500 DEG C, make the p- of 60 ~ 300 mesh
Zsm-5 catalyst intermediate.h3po4The concentration of solution is 4 weight %, and the weight of solution and molecular sieve ratio is for 2:1.Zsm-5 molecule
The mass ratio of sieve and matrix is 3:7；The silicoaluminophosphate molecular of zsm-5 molecular sieve is than for 32；Matrix is kaolin and alundum (Al2O3)
Mixture, both mass ratioes are 7:3.By mg mass of ion percentage composition be 2%, zn mass of ion percentage composition be 3% molten
Liquid, is impregnated with solution and p-zsm-5 catalyst weight than for 1:1, at 120 DEG C be dried 5 hours, place into Muffle furnace in
Roasting 6 hours at 550 DEG C, being prepared into zn constituent content is 2.86 weight %, and mg constituent content is 1.9 weight %, and p element content is
The zn-mg-p-zsm-5 catalyst of 2.35 weight %.
Table 1
| Yield of ethene, weight % | Propene yield, weight % | Aromatics yield, weight % | |
| Embodiment 1 | 28.3 | 25.4 | 34.9 |
| Embodiment 2 | 13.6 | 10.2 | 63.7 |
| Embodiment 3 | 29.2 | 19.4 | 28.9 |
| Embodiment 4 | 15.0 | 10.2 | 64.4 |
| Embodiment 5 | 14.1 | 11.5 | 66.4 |
| Embodiment 6 | 18.8 | 16.5 | 58.1 |
| Embodiment 7 | 15.7 | 13.1 | 62.6 |
| Embodiment 8 | 20.4 | 18.7 | 48.3 |
Claims (9)
1. the system of a kind of methyl alcohol and/or dimethyl ether conversion ethene, propylene and aromatic hydrocarbons, including reactor (1), reactor
(2), regenerator (3), stripper (4), methyl alcohol and/or dimethyl ether (7), recycle stock (8) are respectively in reactor (1), reactor
(2) catalyst neutralisation haptoreaction, reacted carbon deposited catalyst enters stripper (4), the carbon deposited catalyst after stripping
Enter regenerator (3) regeneration through regenerator sloped tube (13), the catalyst after regeneration is through regenerator sloped tube (5), regenerator sloped tube (6)
Respectively enter reactor (1), reactor (2)；
Methyl alcohol and/or dimethyl ether are converted into based on ethene, propylene and aromatic hydrocarbons in reactor (1) catalyst neutralisation haptoreaction
Product；Recycle stock is converted into based on ethene, propylene and aromatic hydrocarbons in reactor (2) catalyst neutralisation haptoreaction
Product；Carbon deposited catalyst is stripped off the product carrying in stripper (4)；Carbon deposited catalyst leads in regenerator (3)
Cross the mode burnt and remove coke.
2. a kind of method of methyl alcohol and/or dimethyl ether conversion ethene, propylene and aromatic hydrocarbons, using the system described in claim 1,
Described method includes following step；
A), in reactor (1) catalyst neutralisation haptoreaction, recycle stock (8) is in reactor for methyl alcohol and/or dimethyl ether (7)
(2) catalyst neutralisation haptoreaction, reaction of formation product and carbon deposited catalyst enter stripper (4) and stripping fluid (10)
Contact, obtains product (9) and carbon deposited catalyst；
B) carbon deposited catalyst enters regenerator (3) through regenerator sloped tube (13)；
C) carbon deposited catalyst burns in regenerator (3) neutralization regenerating medium (11) contact, obtains catalyst and flue gas (12)；
D) catalyst respectively enters reactor (1), reactor (2) through regenerator sloped tube (5), regenerator sloped tube (6)；
E) product (9) enters subsequent separation system, part ethane, propane, c4 and c5 and c6 non-aromatic conduct circulation in product
Material (8) proceeds to react, and remaining product using ethene, propylene, BTX aromatics based on is as output of products system.
3. the method for methyl alcohol according to claim 2 and/or dimethyl ether conversion ethene, propylene and aromatic hydrocarbons, its feature exists
Reaction temperature in reactor is 400～550 DEG C, counts reaction pressure for 0～0.5 MPa with gauge pressure, and weight space velocity is 2～10
(Grams Per Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and methyl alcohol and/or dimethyl ether inlet amount is 3～30: 1, reaction
In device, density of catalyst is 50～150 kgs/m3, average gas superficial velocity 0.7～5 meter per second.
4. the method for methyl alcohol according to claim 2 and/or dimethyl ether conversion ethene, propylene and aromatic hydrocarbons, its feature exists
Reaction temperature in reactor is 430～650 DEG C, counts reaction pressure for 0～0.5 MPa with gauge pressure, and weight space velocity is 2～20
(Grams Per Hour)/gram catalyst, the mass ratio of catalyst internal circulating load and recycle stock inlet amount is catalysis in 5～40: 1, reactor
Agent density is 50～150 kgs/m3, average gas superficial velocity 0.7～7 meter per second.
5. the method for methyl alcohol according to claim 2 and/or dimethyl ether conversion ethene, propylene and aromatic hydrocarbons, its feature exists
It is the composite molecular screen that zsm-5, zsm-23, zsm-11, β, y or mutual are formed in the active component of catalyst；Carrier is height
Ridge soil, aluminum oxide, silica；The mass ratio of active component and carrier is (10～50): (50～90).
6. the method for methyl alcohol according to claim 2 and/or dimethyl ether conversion ethene, propylene and aromatic hydrocarbons, its feature exists
It is loaded with one or more element or oxide in zn, ag, p, ga, cu, mn, mg in catalyst, with the percent mass of catalyst
Ratio meter, its content is 0.01～15 weight %.
7. the method for methyl alcohol according to claim 2 and/or dimethyl ether conversion ethene, propylene and aromatic hydrocarbons, its feature exists
It is methyl alcohol or dimethyl ether or both mixtures in raw material, in raw material, the weight/mass percentage composition of water is 0～30 weight %.
8. the method for methyl alcohol according to claim 2 and/or dimethyl ether conversion ethene, propylene and aromatic hydrocarbons, its feature exists
It is water vapour, n in stripping fluid (10)2Or both mixtures, regenerating medium (11) is air, o2、n2Or both or three
Mixture.
9. the method for methyl alcohol according to claim 2 and/or dimethyl ether conversion ethene, propylene and aromatic hydrocarbons, its feature exists
The percentage composition that coke on catalyst accounts for catalyst gross mass is less than 0.1 weight %.
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| CN101279872A (en) * | 2007-04-04 | 2008-10-08 | 中国石油化工股份有限公司 | Method for preparing low-carbon olefin hydrocarbon with oxocompound |
| CN102875299A (en) * | 2011-07-12 | 2013-01-16 | 中国石油化工股份有限公司 | Method for producing low-carbon olefins by using methanol and naphtha |
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| CN101279872A (en) * | 2007-04-04 | 2008-10-08 | 中国石油化工股份有限公司 | Method for preparing low-carbon olefin hydrocarbon with oxocompound |
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