CN107540495A - Methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene - Google Patents
Methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene Download PDFInfo
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Abstract
The present invention relates to a kind of methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene, mainly solve that regenerator temperature is higher in production process, make the gradual hydrothermal deactivation of catalyst, aromatics yield reduces, the problem of influenceing device continuous and steady operation.Recirculating fluidized bed reaction-regeneration system of the invention by using double strippers, methanol and/or dimethyl ether contact the technical scheme of generation low-carbon alkene and the effluent rich in aromatic hydrocarbons by fluidized-bed reactor with one or more metal supported catalysts, preferably resolve methanol or dimethyl ether production aromatic hydrocarbons and low-carbon alkene during catalyst hydrothermal deactivation, continuous and steady operation the problem of, available for methanol or dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene industrial production in.
Description
Technical field
The present invention relates to a kind of methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene.Specifically, it is related to
A kind of recirculating fluidized bed reaction-regeneration system that aromatic hydrocarbons and low-carbon alkene are produced by methanol or dimethyl ether.
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, at present, is mainly produced using petroleum path.In recent years, International Crude Oil is high always
Position operation, the production technology to petroleum path bring very big cost pressure.
All the time, coal or producing synthesis gas from natural gas, synthesising gas systeming carbinol and alkene, separation technologies for aromatics have rule
Modelling mature experience, but it is the breakpoint and difficult point of this industrial chain by the process of methanol to ethene, propylene and aromatic hydrocarbons, and be somebody's turn to do
The solution of key technology can provide a new original to produce basic organic ethene, propylene and aromatic hydrocarbons by non-oil resource
Expect route
In various existing methanol, dimethyl ether catalysis transformation technology, the product of methanol/dimethyl ether conversion aromatic hydrocarbons is simultaneously
Including ethene, propylene and aromatic hydrocarbons.The technology initially sees Chang of Mobil companies in 1977 et al. (Journal of
Catalysis, 1977,47,249) report methanol and its oxygenatedchemicals conversion preparation virtue on ZSM-5 molecular sieve catalyst
The method of the hydrocarbons such as hydrocarbon.1985, Mobil companies disclosed first in its United States Patent (USP) applied US1590321
The result of study of methanol, dimethyl ether conversion aromatic hydrocarbons, the research use the phosphorous ZSM-5 molecular sieve for 2.7% (weight) to urge
Agent, reaction temperature are 400~450 DEG C, methanol, dimethyl ether air speed 1.3 (Grams Per Hour)/gram catalyst.
The relevant report and patent in the field are more, but the purpose product of most of technologies is aromatic hydrocarbons, ethene, propylene category
It is low in accessory substance, yield.Such as the patent in terms of methanol 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 methanol aromatics process
Patent：United States Patent (USP) US4686312, Chinese patent ZL101244969, ZL1880288, CN101602646,
CN101823929, CN101671226, CN102199069, CN102199446, CN1880288 etc..
In addition, while technology path disclosed in some patents is methanol aromatic hydrocarbons co-producing light olefins, gasoline etc. other
Product, such as patent CN102775261, CN102146010, CN102531821, CN102190546, CN102372537.
Wherein, Multi-function methanol processing method disclosed in patent CN102775261 and device utilize methanol production low-carbon alkene
Hydrocarbon, gasoline, aromatic hydrocarbons.This method uses two-step method production technology, and first step methanol feedstock produces low under the effect of special-purpose catalyst 1
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
Synthesize aromatic hydrocarbons and/or gasoline.The reactor of two courses of reaction can be fixed bed or fluid bed.This method uses two-step method, technique
Flow is complicated.
Patent CN102146010 discloses the work that low-carbon alkene and arene parallel cogeneration gasoline are produced using methanol as raw material
Skill.Low-carbon alkene and aromatic hydrocarbons are produced using methanol as raw material and using molecular sieve catalyst through methanol alkylation reaction and aromatization
Co-production gasoline.The reactor of methanol 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).This method is also adopted
It is complicated with two reactors, technological process.
Patent CN102531821 discloses methanol and the method for the co-feeding production low-carbon alkene of naphtha and/or aromatic hydrocarbons,
Using load 2.2~6.0% (weight) La and 1.0~2.8% (weight) P ZSM-5 catalyst, fixed bed reactors can be used
Or fluidized-bed reactor.Reaction temperature is 550~670 DEG C, air speed 1.0~5 (Grams Per Hour)/gram catalyst.The triolefin of this method
Yield is higher, but BTX yields are 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 developed on the basis of preparing propylene by methanol transformation technology, and propylene is main purpose product, and aromatics yield is relatively low.
The above-mentioned existing fluidization that aromatic hydrocarbons is produced using methanol and/or dimethyl ether as raw material all regenerates system using single
System carries out catalyst circular response regeneration.For guarantee high activity of catalyst, it is necessary to which the carbon content of regenerated catalyst is as far as possible low,
0.5% (weight) below, therefore unavoidably needs high temperature regeneration, and general regeneration temperature is more than 650 DEG C.Except reclaimable catalyst
Hydrogen In The Coke and oxygen reaction can produce vapor, and reclaimable catalyst also carries micro vapor secretly.For molecular sieve catalyst,
Activity can be lost because of framework of molecular sieve dealuminzation under this high temperature, hydro-thermal atmosphere, this inactivation is permanent and irreversible.It is right
In current regenerative system, in order to ensure the reproduction quality of catalyst, residence time of the catalyst in regenerator is longer, causes
Catalyst hydrothermal deactivation is serious, and service life reduces, and aromatics yield declines, production cost increase.
The content of the invention
The technical problems to be solved by the invention are that regenerator temperature is higher in the prior art, lose the gradual hydro-thermal of catalyst
Living, aromatics yield reduces, the problem of influenceing device continuous and steady operation, there is provided a kind of methanol or dimethyl ether conversion production aromatic hydrocarbons and
The method of low-carbon alkene.The vapor that this method is carried secretly using double stripper Removal of catalyst, using lower temperature, not exclusively again
Raw burn hydrogen, higher temperature, oxygen-enriched regeneration completely are made charcoal, have the catalyst hydrothermal stability for keeping good, obtain high quality
Low-carbon regenerative agent, improve aromatics yield the advantages of.
In order to solve the above technical problems, the technical solution adopted by the present invention is as follows：A kind of methanol or dimethyl ether conversion production
The method of aromatic hydrocarbons and low-carbon alkene, using recirculating fluidized bed reaction-regeneration system, methanol and/or dimethyl ether are anti-by fluid bed
Device is answered to contact generation low-carbon alkene and the effluent rich in aromatic hydrocarbons with one or more metal supported catalysts；It is characterized in that institute
Recirculating fluidized bed reaction-regeneration system includes fluidized-bed reactor (1), reactor heat collector (4), reactor cyclonic separation
Device (5), the first stripper (6), inclined tube (7) to be generated, riser (8) to be generated, thick cyclone separator (9), settler (10), second
Stripper (12), settler cyclone separator (13), inclined tube (14) to be generated, first fluidized bed regenerator (15), regenerator whirlwind
Separator (18), external catalyst cooler for regenerator (19), macroporous plate (20), second fluidized bed regenerator (21), outer circulating tube (22),
Degassing tank (23) and regenerator sloped tube (24)；The reclaimable catalyst of inactivation strips the micro hydrocarbon of the entrainment in removing spent agent through two-stage
After class and vapor, in first fluidized bed regenerator, annealing in hydrogen atmosphere process is mainly completed using lower temperature, subsequently into the second fluidisation
Bed regenerator controls higher temperature to complete to make charcoal, the regenerated catalyst of obtained high quality.
In above-mentioned technical proposal, it is preferable that metal supported catalyst is silica alumina ratio SiO2/Al2O3At least 10~100
Crystal aluminosilicate.
In above-mentioned technical proposal, it is highly preferred that catalyst is loaded with least one of Zn, Ag, P, Ga, Cu, Mn and Mg member
Element or oxide.
In above-mentioned technical proposal, it is preferable that crystal aluminosilicate is ZSM-5 and/or ZSM-11.
In above-mentioned technical proposal, it is preferable that carried metal is preferably Zn and/or Sb；It is highly preferred that Zn and Sb weight ratio
For (1：9)~(1：4).
In technical scheme, carried metal mainly exists in the form of the oxide in the catalyst, works as catalyst
When being expressed as a%Zn/ZSM-5, the mass percentage content for illustrating Zn elements in catalyst is a%, except Zn or its oxide
Remaining is ZSM-5 outside, contains other trace elements in catalyst because raw material or other reasonses ultimately result in preparation process
The general component for being not counted in catalyst.
In above-mentioned technical proposal, it is preferable that the regenerated catalyst carbon content is less than 0.1%.
In above-mentioned technical proposal, it is preferable that fluidized-bed reactor (1), settler (10) and first fluidized bed regenerator
(15) it is arranged in juxtaposition.
In above-mentioned technical proposal, it is preferable that methanol or dimethyl ether conversion reaction use turbulent fluid bed reactor (1), wrap
Emulsion zone (2) and dilute-phase zone (3) are included, methanol or dimethyl ether enter emulsion zone (2) and catalyst from fluidized-bed reactor (1) bottom
Contact carries out the reaction generation product such as aromatic hydrocarbons and low-carbon alkene, the reactor that the product gas of entrained catalyst passes through dilute-phase zone (3)
Fluidized-bed reactor (1) is left after cyclone separator (5) progress gas solid separation and enters subsequent separation system, and the catalyst of recovery returns
Return emulsion zone (2).
In above-mentioned technical proposal, it is preferable that reclaimable catalyst sets two before first fluidized bed regenerator (15) is entered
Stripper, by the catalyst inclined tube to be generated (7) of inactivation, riser (8) to be generated and settler (10) join the first stripper (6)
Logical, settler (10) includes settling section (11) and the second stripper (section) (12), and interior structure is may also set up in the second stripper (12)
Part strengthens Srteam Stripping effect, and general steam stripping efficiency is both greater than 85%.
In above-mentioned technical proposal, it is preferable that the reclaimable catalyst of inactivation first passes through the first stripper, using inert media
(25) after removing micro hydro carbons, by inclined tube to be generated (7), riser (8) to be generated, thick cyclone separator (9) enter the second stripping
Device (12), using the vapor of the entrainment in nitrogen or air (26) removing spent agent, reduction enters first fluidized bed regenerator
(15) steam vapour amount, the hydrothermal deactivation degree of catalyst is reduced, improves the stability of catalyst.By nitrogen or air (26)
Reclaimable catalyst after stripping enters first fluidized bed regenerator (15) by inclined tube to be generated (14)；It is highly preferred that inert media
(25) it is high steam.
In above-mentioned technical proposal, it is preferable that catalyst regeneration is regenerated using two sections of turbulent fluidized bed regenerators, including first
Fluid bed regenerator (15), first fluidized bed regenerator emulsion zone (16), first fluidized bed regenerator dilute-phase zone (17) and regeneration
Device cyclone separator (18), external catalyst cooler for regenerator (19), second fluidized bed regenerator (21) and macroporous plate (20)；More preferably
Ground, regenerator cyclone separator (18) are 1-5 levels, generally 2 or 3 grades.
In above-mentioned technical proposal, it is preferable that methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene, its feature
Be first fluidized bed regenerator (15) above, second fluidized bed regenerator (21) below, second fluidized bed regenerator
(21) top insertion first fluidized bed regenerator (15) bottom, both pass through macroporous plate (20) and semi regeneration outer circulating tube (22)
Connection.
In above-mentioned technical proposal, it is preferable that reclaimable catalyst is in first fluidized bed regenerator (15) emulsion zone (16) and one
Air (28) contact again carries out catalyst regeneration.First fluidized bed regenerator (15) is based on annealing in hydrogen atmosphere, using relatively low regeneration temperature
Degree and appropriate oxygen content carry out incomplete regen-eration, control oxygen content in flue gas to be less than 1%.First fluidized bed regenerator
(15) the semi regeneration catalyst in enters second fluidized bed regenerator (21) bottom, second by semi regeneration outer circulating tube (22)
Change bed regenerator (21) based on making charcoal, the higher regeneration temperature of use, oxygen-enriched regeneration completely, obtain the low-carbon regeneration of high quality
Agent.
In above-mentioned technical proposal, it is preferable that methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene, its feature
It is that main wind (29) enters oxygen content excessive two from second fluidized bed regenerator (21) bottom again and semi regeneration catalyst is in high temperature
Under the conditions of, regenerated completely；Flue gas enters the first fluidized bed again to two of oxygen content more than 1% by macroporous plate (20) again
Raw device (15) emulsion zone (16) mixes with main wind (28) again and again, is carried out not with the reclaimable catalyst from fluidized-bed reactor (1)
Regeneration completely.Flue gas of the oxygen content less than 1% reclaims catalyst by the regenerator cyclone separator (18) of dilute-phase zone (17)
Afterwards, leave fluid bed regenerator (15) and enter subsequent power recovery system.
In above-mentioned technical proposal, it is preferable that fluidized-bed reactor (1) is by setting interior heat collector (4) or external warmer (4)
Or set interior heat collector (4) and external warmer (4) to remove heat caused by reaction simultaneously, while control fluidized-bed reactor (1)
Reaction temperature.The reclaimable catalyst of fluidized-bed reactor (1) interior carbon deposit is after stripper (6) removes micro hydro carbons, through treating
Raw inclined tube (7), riser to be generated (8), thick cyclone separator (9) are sent into settler (10)；It is highly preferred that lifting gas (21) is height
Press steam.
In above-mentioned technical proposal, it is preferable that the high temperature catalyst in first fluidized bed regenerator (15) outside device by taking
Hot device (19) returns to first fluidized bed regenerator (15) emulsion zone (16) after reducing temperature, by controlling catalyst internal circulating load to adjust
Save first fluidized bed regenerator (15) regeneration temperature；The catalyst regenerated completely in second fluidized bed regenerator (21) is by degassing
After the micro non-hydrocarbon gases of tank (23) Removal of catalyst entrainment, enter fluidized-bed reactor (1) close phase through regenerator sloped tube (24)
Area (2).
In above-mentioned technical proposal, it is preferable that methanol or 400~550 DEG C of the reaction temperature of dimethyl ether conversion reaction, reaction pressure
0~1.0MPa of power, 200~550 kgs/m of reactor emulsion zone (2) catalyst averag density3, it is empty in fluidized-bed reactor (1)
The meter per second of tower linear speed 0.1~1.0.
In above-mentioned technical proposal, it is preferable that 500~600 DEG C of first fluidized bed regenerator (15) regeneration temperature, regeneration pressure
0~1.0MPa, 150~550 kgs/m of emulsion zone (16) catalyst averag density3, first fluidized bed regenerator emulsion zone (16)
The interior meter per second of void tower linear speed 0.1~1.0.
In above-mentioned technical proposal, it is preferable that 600~720 DEG C of second fluidized bed regenerator (21) regeneration temperature, regeneration pressure
0~1.2MPa, 150~550 kgs/m of catalyst averag density3, the interior void tower linear speed 0.1 of second fluidized bed regenerator (21)~
1.0 meter per second.
For methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene, it is proposed that recirculating fluidized bed reaction-again
Raw system is by fluidized-bed reactor (1), reactor external warmer (4), reactor cyclone (5), the first stripper (6),
Inclined tube (7) to be generated, riser (8) to be generated, thick cyclone separator (9), settler (10), the second stripper (12), settler rotation
Wind separator (13), inclined tube (14) to be generated, first fluidized bed regenerator (15), regenerator cyclone separator (18), outside regenerator
Heat collector (19), second fluidized bed regenerator (21), semi regeneration outer circulating tube (22), degassing tank (23), regenerator sloped tube (24) and
The structures such as macroporous plate (20), are shown in accompanying drawing 1, Fig. 2.Using technical scheme, burnt by low regeneration temperature, incomplete regen-eration
Hydrogen, higher regeneration temperature, oxygen-enriched regeneration completely are made charcoal, have the catalyst hydrothermal stability for keeping good simultaneously, obtain high-quality
The low-carbon regenerative agent of amount, carbon content is less than 0.1% on regenerated catalyst, maintains higher aromatics yield, its aromatic hydrocarbons it is carbon-based
Yield achieves good technique effect up to more than 60%.
Brief description of the drawings
Fig. 1 is recirculating fluidized bed reaction-regeneration system system of the present invention (fluidized-bed reactor setting interior heat collector) signal
Figure；
Fig. 2 is recirculating fluidized bed reaction-regeneration system system of the present invention (fluidized-bed reactor setting external warmer) signal
Figure；
In Fig. 1 or Fig. 2,1 is fluidized-bed reactor；2 be reactor emulsion zone, and 3 be reactor dilute-phase zone；4 be reaction
Device external warmer；5 be reactor cyclone；6 be the first stripper；7 be inclined tube to be generated；8 be riser to be generated；9 be thick
Cyclone separator；10 be settler；11 be settling section；12 be the second stripper (section)；13 be settler cyclone separator；14 are
Inclined tube to be generated；15 be first fluidized bed regenerator；16 be first fluidized bed regenerator emulsion zone；17 be first fluidized bed regenerator
Dilute-phase zone；18 be regenerator cyclone separator；19 be external catalyst cooler for regenerator；20 be macroporous plate；21 be second fluidized bed again
Raw device；22 be semi regeneration outer circulating tube；23 be degassing tank；24 be regenerator sloped tube, and 25 be stripping vapor；26 for stripping air or
Nitrogen；27 be lifting gas；28 be the main wind of first fluidized bed regenerator (main wind again and again)；29 be the main wind of second fluidized bed regenerator
(two again main wind).
Below by embodiment, the invention will be further elaborated.
Specific embodiment
【Embodiment 1】
The device of 1800000 tons/year of methanol production aromatic hydrocarbons and low-carbon alkene using recirculating fluidized bed as shown in Figure 1 reaction-again
Raw system.Fluidized-bed reactor sets interior heat collector, anti-using metal supported catalyst 1%Zn/3%La/ZSM-5, fluid bed
The reaction process condition for answering device is：Reaction temperature is 450 DEG C, reaction pressure 0.3MPa, emulsion zone catalyst averag density 300
Kg/m3, the average meter per second of void tower linear speed 0.7.The technological condition of regeneration of fluid bed regenerator is：Again and again temperature be 550 DEG C, one
Pressure is 0.2MPa again, again and again 300 kgs/m of emulsion zone catalyst averag density3, the average meter per second of void tower linear speed 0.8 again and again；
Two again temperature be 680 DEG C, two again pressure be 0.21MPa, two 450 kgs/m of emulsion zone catalyst averag density again3, put down again and again
The equal meter per second of void tower linear speed 0.5, two main wind oxygen content 21% (volume) again, exhanst gas outlet oxygen content 0.8% (volume) again and again, two
Exhanst gas outlet oxygen content 5% (volume) again, carbon content 0.05% on regenerated catalyst, the stripper efficiency of the second stripper
91%.
Under conditions above and structural parameters, methanol aromatic hydrocarbons and alkene are carried out by method of the present invention, can obtain
More satisfactory result, aromatic hydrocarbons carbon base absorption rate 60.92%, ethene carbon base absorption rate 7.85%, propylene carbon base absorption rate 6.46%.
【Embodiment 2】
The device of 1200000 tons/year of methanol production aromatic hydrocarbons and low-carbon alkene using recirculating fluidized bed as shown in Figure 1 reaction-again
Raw system.Fluidized-bed reactor sets interior heat collector, anti-using metal supported catalyst 1%Zn/3%La/ZSM-5, fluid bed
The reaction process condition for answering device is：Reaction temperature is 480 DEG C, reaction pressure 0.3MPa, emulsion zone catalyst averag density 380
Kg/m3, the average meter per second of void tower linear speed 0.8.The technological condition of regeneration of fluid bed regenerator is：Again and again temperature be 530 DEG C, one
Pressure is 0.3MPa again, again and again 350 kgs/m of emulsion zone catalyst averag density3, the average meter per second of void tower linear speed 0.6 again and again；
Two again temperature be 690 DEG C, two again pressure be 0.31MPa, two 350 kgs/m of emulsion zone catalyst averag density again3, put down again and again
The equal meter per second of void tower linear speed 0.8, two main wind oxygen content 21% (volume) again, exhanst gas outlet oxygen content 0.5% (volume) again and again, two
Exhanst gas outlet oxygen content 2.3% (volume) again, carbon content 0.04% on regenerated catalyst, the stripper efficiency of the second stripper
95%.
Under conditions above and structural parameters, methanol aromatic hydrocarbons and alkene are carried out by method of the present invention, can obtain
More satisfactory result, aromatic hydrocarbons carbon base absorption rate 62.51%, ethene carbon base absorption rate 8.07%, propylene carbon base absorption rate 6.38%.
【Embodiment 3】
The device of 1800000 tons/year of methanol production aromatic hydrocarbons and low-carbon alkene using recirculating fluidized bed as shown in Figure 2 reaction-again
Raw system, fluidized-bed reactor sets external warmer, using metal supported catalyst 1%Zn/3%La/ZSM-5.Using Zn-
Mg-ZSM-5 catalyst, the reaction process condition of fluidized-bed reactor are：Reaction temperature is 490 DEG C, reaction pressure 0.2MPa,
430 kgs/m of emulsion zone catalyst averag density3, the average meter per second of void tower linear speed 0.9.The regeneration technology bar of fluid bed regenerator
Part is：Temperature is 560 DEG C again and again, and pressure is 0.2MPa again and again, again and again 250 kgs/m of emulsion zone catalyst averag density3, one
Be averaged the meter per second of void tower linear speed 0.8 again；Two again temperature be 680 DEG C, two again pressure be 0.21MPa, two again emulsion zone catalyst be averaged
380 kgs/m of density3, the average meter per second of void tower linear speed 0.7 again and again, two main wind oxygen content 21% (volume) again, flue gas goes out again and again
Suck oxygen amount 0.9% (volume), two exhanst gas outlet oxygen content 4.3% (volumes) again, carbon content 0.07% on regenerated catalyst,
The stripper efficiency 88% of second stripper.
Under conditions above and structural parameters, methanol aromatic hydrocarbons and alkene are carried out by method of the present invention, can obtain
More satisfactory result, aromatic hydrocarbons carbon base absorption rate 63.26%, ethene carbon base absorption rate 6.3%, propylene carbon base absorption rate 4.89%.
【Embodiment 4】
The device of 600000 tons/year of methanol production aromatic hydrocarbons and low-carbon alkene using recirculating fluidized bed as shown in Figure 2 reaction-again
Raw system, fluidized-bed reactor sets external warmer, using metal supported catalyst 1%Zn/3%La/ZSM-5.Fluid bed is anti-
The reaction process condition for answering device is：Reaction temperature is 470 DEG C, reaction pressure 0.5MPa, emulsion zone catalyst averag density 300
Kg/m3, the average meter per second of void tower linear speed 0.6.The technological condition of regeneration of fluid bed regenerator is：Again and again temperature be 550 DEG C, one
Pressure is 0.5MPa again, again and again 200 kgs/m of emulsion zone catalyst averag density3, 0.9 meter of the void tower linear speed that is averaged again and again/
Second；Two again temperature be 670 DEG C, two again pressure be 0.51MPa, two 350 kgs/m of emulsion zone catalyst averag density again3, again and again
The average meter per second of void tower linear speed 0.8, two main wind oxygen content 21% (volume) again, exhanst gas outlet oxygen content 0.6% (volume) again and again,
Two exhanst gas outlet oxygen content 3.6% (volumes) again, carbon content 0.06% on regenerated catalyst, the stripper effect of the second stripper
Rate 90%.
Under conditions above and structural parameters, methanol aromatic hydrocarbons and alkene are carried out by method of the present invention, can obtain
More satisfactory result, aromatic hydrocarbons carbon base absorption rate 63.3%, ethene carbon base absorption rate 6.17%, propylene carbon base absorption rate 4.94%.
【Embodiment 5】
The device of 1800000 tons/year of methanol production aromatic hydrocarbons and low-carbon alkene using recirculating fluidized bed as shown in Figure 1 reaction-again
Raw system, fluidized-bed reactor sets interior heat collector, using metal supported catalyst 1%Zn/3%La/ZSM-5.Fluid bed is anti-
The reaction process condition for answering device is：Reaction temperature is 480 DEG C, reaction pressure 0.15MPa, emulsion zone catalyst averag density
480 kgs/m3, the average meter per second of void tower linear speed 0.5.The technological condition of regeneration of fluid bed regenerator is：Temperature is 550 again and again
DEG C, pressure is 0.15MPa again and again, again and again 320 kgs/m of emulsion zone catalyst averag density3, be averaged void tower linear speed again and again
0.7 meter per second；Two again temperature be 660 DEG C, two again pressure be 0.16MPa, two 400 kgs/m of emulsion zone catalyst averag density again
3, the average meter per second of void tower linear speed 0.6 again and again, two main wind oxygen content 21% (volume) again, exhanst gas outlet oxygen content 0.8% again and again
(volume), two exhanst gas outlet oxygen content 6% (volumes) again, carbon content 0.08% on regenerated catalyst, the vapour of the second stripper
Put forward device efficiency 93%.
Under conditions above and structural parameters, methanol aromatic hydrocarbons and alkene are carried out by method of the present invention, can obtain
More satisfactory result, aromatic hydrocarbons carbon base absorption rate 62.78%, ethene carbon base absorption rate 7.1%, propylene carbon base absorption rate 5.47%.
【Embodiment 6】
The device of 1200000 tons/year of methanol production aromatic hydrocarbons and low-carbon alkene using recirculating fluidized bed as shown in Figure 2 reaction-again
Raw system, fluidized-bed reactor sets external warmer, using metal supported catalyst 1%Zn/3%La/ZSM-5.Fluid bed is anti-
The reaction process condition for answering device is：Reaction temperature is 500 DEG C, reaction pressure 0.05MPa, emulsion zone catalyst averag density
550 kg/m 3, the average meter per second of void tower linear speed 0.8.The technological condition of regeneration of fluid bed regenerator is：Temperature is 530 again and again
DEG C, pressure is 0.05MPa again and again, again and again 350 kgs/m of emulsion zone catalyst averag density3, be averaged void tower linear speed again and again
0.6 meter per second；Two again temperature be 690 DEG C, two again pressure be 0.06MPa, two 350 kgs/m of emulsion zone catalyst averag density again
3, the average meter per second of void tower linear speed 0.8 again and again, two main wind oxygen content 21% (volume) again, exhanst gas outlet oxygen content 0.5% again and again
(volume), two exhanst gas outlet oxygen content 4.3% (volumes) again, carbon content 0.08% on regenerated catalyst, the second stripper
Stripper efficiency 96%.
Under conditions above and structural parameters, methanol aromatic hydrocarbons and alkene are carried out by method of the present invention, can obtain
More satisfactory result, aromatic hydrocarbons carbon base absorption rate 53.83%, ethene carbon base absorption rate 14.02%, propylene carbon base absorption rate 10.17%.
【Embodiment 7】
The device of 1800000 tons/year of methanol production aromatic hydrocarbons and low-carbon alkene using recirculating fluidized bed as shown in Figure 1 reaction-again
Raw system, fluidized-bed reactor sets interior heat collector, using metal supported catalyst 1%Zn/3%Cs/ZSM-11.Fluid bed is anti-
The reaction process condition for answering device is：Reaction temperature is 480 DEG C, reaction pressure 0.15MPa, emulsion zone catalyst averag density
480 kgs/m3, the average meter per second of void tower linear speed 0.5.The technological condition of regeneration of fluid bed regenerator is：Temperature is 550 again and again
DEG C, pressure is 0.15MPa again and again, again and again 320 kgs/m of emulsion zone catalyst averag density3, be averaged void tower linear speed again and again
0.7 meter per second；Two again temperature be 660 DEG C, two again pressure be 0.16MPa, two 400 kgs/m of emulsion zone catalyst averag density again
3, the average meter per second of void tower linear speed 0.6 again and again, two main wind oxygen content 21% (volume) again, exhanst gas outlet oxygen content 0.8% again and again
(volume), two exhanst gas outlet oxygen content 6% (volumes) again, carbon content 0.08% on regenerated catalyst, the vapour of the second stripper
Put forward device efficiency 93%.
Under conditions above and structural parameters, methanol aromatic hydrocarbons and alkene are carried out by method of the present invention, can obtain
More satisfactory result, aromatic hydrocarbons carbon base absorption rate 62.50%, ethene carbon base absorption rate 7.5%, propylene carbon base absorption rate 5.8%.
【Embodiment 8】
The device of 1800000 tons/year of methanol production aromatic hydrocarbons and low-carbon alkene using recirculating fluidized bed as shown in Figure 1 reaction-again
Raw system, fluidized-bed reactor sets interior heat collector, using metal supported catalyst 1%Zn/3%La/SBA-15.Fluid bed is anti-
The reaction process condition for answering device is：Reaction temperature is 480 DEG C, reaction pressure 0.15MPa, emulsion zone catalyst averag density
480 kgs/m3, the average meter per second of void tower linear speed 0.5.The technological condition of regeneration of fluid bed regenerator is：Temperature is 550 again and again
DEG C, pressure is 0.15MPa again and again, again and again 320 kgs/m of emulsion zone catalyst averag density3, be averaged void tower linear speed again and again
0.7 meter per second；Two again temperature be 660 DEG C, two again pressure be 0.16MPa, two 400 kgs/m of emulsion zone catalyst averag density again
3, the average meter per second of void tower linear speed 0.6 again and again, two main wind oxygen content 21% (volume) again, exhanst gas outlet oxygen content 0.8% again and again
(volume), two exhanst gas outlet oxygen content 6% (volumes) again, carbon content 0.08% on regenerated catalyst, the vapour of the second stripper
Put forward device efficiency 93%.
Under conditions above and structural parameters, methanol aromatic hydrocarbons and alkene are carried out by method of the present invention, can obtain
More satisfactory result, aromatic hydrocarbons carbon base absorption rate 60.5%, ethene carbon base absorption rate 6.8%, propylene carbon base absorption rate 6.6%.
【Embodiment 9】
The device of 1200000 tons/year of methanol production aromatic hydrocarbons and low-carbon alkene using recirculating fluidized bed as shown in Figure 2 reaction-again
Raw system, fluidized-bed reactor sets external warmer, using metal supported catalyst 1%Zn/3%Sb/ZSM-5.Fluid bed is anti-
The reaction process condition for answering device is：Reaction temperature is 500 DEG C, reaction pressure 0.05MPa, emulsion zone catalyst averag density
550 kg/m 3, the average meter per second of void tower linear speed 0.8.The technological condition of regeneration of fluid bed regenerator is：Temperature is 530 again and again
DEG C, pressure is 0.05MPa again and again, again and again 350 kgs/m of emulsion zone catalyst averag density3, be averaged void tower linear speed again and again
0.6 meter per second；Two again temperature be 690 DEG C, two again pressure be 0.06MPa, two 350 kgs/m of emulsion zone catalyst averag density again
3, the average meter per second of void tower linear speed 0.8 again and again, two main wind oxygen content 21% (volume) again, exhanst gas outlet oxygen content 0.5% again and again
(volume), two exhanst gas outlet oxygen content 4.3% (volumes) again, carbon content 0.08% on regenerated catalyst, the second stripper
Stripper efficiency 96%.
Under conditions above and structural parameters, methanol aromatic hydrocarbons and alkene are carried out by method of the present invention, can obtain
More satisfactory result, aromatic hydrocarbons carbon base absorption rate 60.5%, ethene carbon base absorption rate 13.2%, propylene carbon base absorption rate 9.8%.
【Embodiment 10】
The device of 1200000 tons/year of methanol production aromatic hydrocarbons and low-carbon alkene using recirculating fluidized bed as shown in Figure 2 reaction-again
Raw system, fluidized-bed reactor sets external warmer, using metal supported catalyst 0.4%Zn/3.6%Sb/ZSM-5.Fluidisation
Bed reactor reaction process condition be：Reaction temperature is 500 DEG C, reaction pressure 0.05MPa, and emulsion zone catalyst is average close
550 kg/m 3 of degree, the average meter per second of void tower linear speed 0.8.The technological condition of regeneration of fluid bed regenerator is：Temperature is 530 again and again
DEG C, pressure is 0.05MPa again and again, again and again 350 kgs/m of emulsion zone catalyst averag density3, be averaged void tower linear speed again and again
0.6 meter per second；Two again temperature be 690 DEG C, two again pressure be 0.06MPa, two 350 kgs/m of emulsion zone catalyst averag density again
3, the average meter per second of void tower linear speed 0.8 again and again, two main wind oxygen content 21% (volume) again, exhanst gas outlet oxygen content 0.5% again and again
(volume), two exhanst gas outlet oxygen content 4.3% (volumes) again, carbon content 0.08% on regenerated catalyst, the second stripper
Stripper efficiency 96%.
Under conditions above and structural parameters, methanol aromatic hydrocarbons and alkene are carried out by method of the present invention, can obtain
More satisfactory result, aromatic hydrocarbons carbon base absorption rate 63.5%, ethene carbon base absorption rate 12.6%, propylene carbon base absorption rate 9.5%.
【Embodiment 11】
The device of 1200000 tons/year of methanol production aromatic hydrocarbons and low-carbon alkene using recirculating fluidized bed as shown in Figure 2 reaction-again
Raw system, fluidized-bed reactor sets external warmer, using metal supported catalyst 0.8%Zn/3.2%Sb/ZSM-5.Fluidisation
Bed reactor reaction process condition be：Reaction temperature is 500 DEG C, reaction pressure 0.05MPa, and emulsion zone catalyst is average close
550 kgs/m of degree3, the average meter per second of void tower linear speed 0.8.The technological condition of regeneration of fluid bed regenerator is：Temperature is 530 again and again
DEG C, pressure is 0.05MPa again and again, again and again 350 kgs/m of emulsion zone catalyst averag density3, be averaged void tower linear speed again and again
0.6 meter per second；Two again temperature be 690 DEG C, two again pressure be 0.06MPa, two 350 kgs/m of emulsion zone catalyst averag density again
3, the average meter per second of void tower linear speed 0.8 again and again, two main wind oxygen content 21% (volume) again, exhanst gas outlet oxygen content 0.5% again and again
(volume), two exhanst gas outlet oxygen content 4.3% (volumes) again, carbon content 0.08% on regenerated catalyst, the second stripper
Stripper efficiency 96%.
Under conditions above and structural parameters, methanol aromatic hydrocarbons and alkene are carried out by method of the present invention, can obtain
More satisfactory result, aromatic hydrocarbons carbon base absorption rate 63.8%, ethene carbon base absorption rate 12.8%, propylene carbon base absorption rate 9.4%.
【Comparative example 1】
The device of 1800000 tons/year of methanol production aromatic hydrocarbons and low-carbon alkene using recirculating fluidized bed as shown in Figure 1 reaction-again
Raw system, fluidized-bed reactor sets interior heat collector, using metal supported catalyst 1%Zn/3%La/ZSM-5.Fluid bed is anti-
The reaction process condition for answering device is：Reaction temperature is 470 DEG C, reaction pressure 0.5MPa, emulsion zone catalyst averag density 330
Kg/m3, the average meter per second of void tower linear speed 0.5.The technological condition of regeneration of fluid bed regenerator is：Again and again temperature be 680 DEG C, one
Pressure is 0.5MPa again, again and again 280 kgs/m of emulsion zone catalyst averag density3, the average meter per second of void tower linear speed 0.7 again and again；
Two again temperature be 680 DEG C, two again pressure be 0.51MPa, two 310 kgs/m of emulsion zone catalyst averag density again3, put down again and again
The equal meter per second of void tower linear speed 0.8, two main wind oxygen content 21% (volume) again, exhanst gas outlet oxygen content 1.8% (volume) again and again, two
Exhanst gas outlet oxygen content 4.1% (volume) again, carbon content 0.08% on regenerated catalyst.
Under conditions above and structural parameters, available operation result, aromatic hydrocarbons carbon base absorption rate 50.95%, the carbon-based receipts of ethene
Rate 13.21%, propylene carbon base absorption rate 9.52%.
【Comparative example 2】
The device of 1800000 tons/year of methanol production aromatic hydrocarbons and low-carbon alkene uses regular circulation fluidized-bed reaction-regeneration system
System, regenerator is one section of regeneration, using metal supported catalyst 1%Zn/3%La/ZSM-5.The reaction work of fluidized-bed reactor
Skill condition is：Reaction temperature is 470 DEG C, reaction pressure 0.5MPa, 300 kgs/m of emulsion zone catalyst averag density3, put down
The equal meter per second of void tower linear speed 0.5.The technological condition of regeneration of fluid bed regenerator is：Temperature is 550 DEG C, regeneration pressure 0.5MPa,
380 kgs/m of regenerator emulsion zone catalyst averag density3, the average meter per second of void tower linear speed 0.6 of regenerator；Main wind oxygen content
21% (volume), exhanst gas outlet oxygen content 0.4% (volume), carbon content 1.8% on regenerated catalyst.
Under conditions above and structural parameters, available operation result, aromatic hydrocarbons carbon base absorption rate 47.71%, the carbon-based receipts of ethene
Rate 16.63%, propylene carbon base absorption rate 11.82%.
Claims (10)
1. a kind of methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene, are reacted-are regenerated using recirculating fluidized bed and be
System, methanol and/or dimethyl ether contact generation low-carbon alkene by fluidized-bed reactor with one or more metal supported catalysts
And the effluent rich in aromatic hydrocarbons；It is characterized in that recirculating fluidized bed reaction-regeneration system used includes fluidized-bed reactor
(1), reactor heat collector (4), reactor cyclone (5), the first stripper (6), inclined tube (7) to be generated, riser to be generated
(8), thick cyclone separator (9), settler (10), the second stripper (12), settler cyclone separator (13), inclined tube to be generated
(14), first fluidized bed regenerator (15), regenerator cyclone separator (18), external catalyst cooler for regenerator (19), macroporous plate
(20), second fluidized bed regenerator (21), outer circulating tube (22), degassing tank (23) and regenerator sloped tube (24)；The to be generated of inactivation is urged
After micro hydro carbons and vapor that agent strips the entrainment in removing spent agent through two-stage, in first fluidized bed regenerator, use
Lower temperature mainly completes annealing in hydrogen atmosphere process, controls higher temperature to complete to make charcoal subsequently into second fluidized bed regenerator, obtains
High quality regenerated catalyst.
2. methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene according to claim 1, it is characterised in that stream
Fluidized bed reactor (1), settler (10) and first fluidized bed regenerator (15) are arranged in juxtaposition.
3. methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene according to claim 1, it is characterised in that first
Alcohol or dimethyl ether conversion reaction use turbulent fluid bed reactor (1), including emulsion zone (2) and dilute-phase zone (3), methanol or diformazan
Ether enters emulsion zone (2) from fluidized-bed reactor (1) bottom and catalyst contact carries out reaction generation aromatic hydrocarbons and low-carbon alkene etc.
Product, the product gas of entrained catalyst pass through dilute-phase zone (3) reactor cyclone (5) carry out gas solid separation after leave stream
Fluidized bed reactor (1) enters subsequent separation system, and the catalyst of recovery returns to emulsion zone (2).
4. methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene according to claim 1, it is characterised in that treat
Raw catalyst sets two strippers, the first stripper (6) urging by inactivation before first fluidized bed regenerator (15) is entered
Agent inclined tube to be generated (7), riser (8) to be generated and settler (10) UNICOM, settler (10) include settling section (11) and second
Stripper (section) (12), the second stripper (12) is interior to may also set up inner member enhancing Srteam Stripping effect, and general steam stripping efficiency is both greater than
85%.
5. methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene according to claim 1, it is characterised in that lose
Reclaimable catalyst living first passes through the first stripper, after removing micro hydro carbons using inert media (25), by inclined tube to be generated
(7), riser (8) to be generated, thick cyclone separator (9) enter the second stripper (12), are treated using nitrogen or air (26) removing
The vapor of entrainment in raw agent, reduces the steam vapour amount into first fluidized bed regenerator (15), reduces the hydro-thermal of catalyst
Level of deactivation, improve the stability of catalyst.Reclaimable catalyst after nitrogen or air (26) stripping passes through inclined tube to be generated
(14) first fluidized bed regenerator (15) is entered.
6. methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene according to claim 1, it is characterised in that urge
Agent regeneration is regenerated using two sections of turbulent fluidized bed regenerators, including the regeneration of first fluidized bed regenerator (15), the first fluidized bed
Device emulsion zone (16), first fluidized bed regenerator dilute-phase zone (17) and regenerator cyclone separator (18), external catalyst cooler for regenerator
(19), second fluidized bed regenerator (21) and macroporous plate (20).
7. methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene according to claim 1, it is characterised in that the
One fluid bed regenerator (15) above, second fluidized bed regenerator (21) below, at the top of second fluidized bed regenerator (21)
First fluidized bed regenerator (15) bottom is inserted, both are connected by macroporous plate (20) with semi regeneration outer circulating tube (22).
8. methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene according to claim 1, it is characterised in that treat
Raw catalyst contacts in first fluidized bed regenerator (15) emulsion zone (16) with air again and again (28) carries out catalyst regeneration.First
Fluid bed regenerator (15) carries out incomplete regen-eration based on annealing in hydrogen atmosphere, using relatively low regeneration temperature and appropriate oxygen content,
Oxygen content in flue gas is controlled to be less than 1%；Semi regeneration catalyst in first fluidized bed regenerator (15) outside semi regeneration by following
Endless tube (22) enters second fluidized bed regenerator (21) bottom, and for second fluidized bed regenerator (21) based on making charcoal, use is higher
Regeneration temperature, it is oxygen-enriched completely regeneration, obtain the low-carbon regenerative agent of high quality.
9. methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene according to claim 1, it is characterised in that contain
Main wind (29) enters with semi regeneration catalyst under the high temperature conditions oxygen amount excessive two from second fluidized bed regenerator (21) bottom again,
Regenerated completely；Flue gas enters first fluidized bed regenerator to two of oxygen content more than 1% by macroporous plate (20) again
(15) emulsion zone (16) mixes with main wind (28) again and again, is carried out with the reclaimable catalyst from fluidized-bed reactor (1) incomplete
Regeneration；After flue gas of the oxygen content less than 1% reclaims catalyst by the regenerator cyclone separator (18) of dilute-phase zone (17), from
Open fluid bed regenerator (15) and enter subsequent power recovery system.
10. methanol or the method for dimethyl ether conversion production aromatic hydrocarbons and low-carbon alkene according to claim 1, it is characterised in that stream
Fluidized bed reactor (1) is by setting interior heat collector (4) or external warmer (4) or setting interior heat collector (4) and external warmer simultaneously
(4) heat caused by reaction is removed, while controls the reaction temperature of fluidized-bed reactor (1)；Fluidized-bed reactor (1) interior carbon deposit
Reclaimable catalyst after stripper (6) removes micro hydro carbons, through inclined tube to be generated (7), riser to be generated (8), thick whirlwind point
Settler (10) is sent into from device (9).
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