CN103752229A - Fixed bed reactor for preparing olefin by oxygen-contained compound - Google Patents
Fixed bed reactor for preparing olefin by oxygen-contained compound Download PDFInfo
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- CN103752229A CN103752229A CN201410038152.0A CN201410038152A CN103752229A CN 103752229 A CN103752229 A CN 103752229A CN 201410038152 A CN201410038152 A CN 201410038152A CN 103752229 A CN103752229 A CN 103752229A
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Abstract
The invention relates to a fixed bed reactor for preparing olefin by an oxygen-contained compound; the fixed bed reactor couples the reaction of preparing propylene/ethylene by catalytic cracking of the olefin and the preparation of propylene/ethylene by the oxygen-contained compound in one reactor, and comprises a feeding opening (1), a discharging opening (20) and a closed container (2); fed materials of the feeding opening (1) are hydrocarbon flows with the temperature of 400.0-650.0 DEG C or water and the hydrocarbon flows; 2-9 catalyst bed layers are sequentially arranged in the closed container from the top to the bottom; inter-section feeding and mixing distributors are arranged between the catalyst bed layers, wherein the fed materials of the uppermost layer of the first inter-section feeding and mixing distributor (4) are water and oxygen-contained compound flows, or water, the oxygen-contained compound and the hydrocarbon flows; the fed materials of the rest inter-section feeding and mixing distributors are water and the oxygen-contained compound. Compared with the prior art, the fixed bed reactor has the advantages of simplicity in reaction, simplicity in construction, easiness in amplification, convenience and flexibility for operation and low investment.
Description
Technical field
The present invention relates to insulation fix bed reactor, particularly the fixed bed reactors of a kind of oxygenatedchemicals alkene processed.
Background technology
Current, ethylene/propene is mainly derived from naphtha and light paraffins steam cracking process, naphtha steam cracking technique relative complex, and cost is higher, and light paraffins steam cracking obtains ethylene/propene, and technique is simple, and cost is lower.Recent year increases gradually to the dependency degree of imported crude oil, and crude oil price also maintains a high position always, and Chinese limited light paraffins resource in addition, in the urgent need to development of new propylene/ethylene production technology.In recent years, China succeeded in developing coal through oxygenatedchemicals as the production technology of preparing propylene from methanol/ethene, and realized the commercial applications of this technology, oxygenatedchemicals alkene technology processed can be divided into fluid bed and bed technology by reactor.
Praxair Technology, Inc (UOP) is at Studies in Surface Science and Catalysis, volume147:p1-6 has openly reported a kind of methanol-to-olefins technology (MTO) that adopts circulating fluid bed reactor and SAPO-34 catalyst, this technology ethylene/propene is selectively 77-78%, by by by-product heavy hydrocarbon (carbon atom be four and above hydrocarbon) through the further preparing propone/ethene of catalyzed conversion (OCP), propylene/ethylene selectively can reach 89.0%, has greatly promoted the raising of propylene/ethylene yield.
Chinese patent CN101367699 discloses the method for the preparing propone of at least two reaction zones of a kind of setting, and wherein, first reaction zone is C
4+hydrocarbon catalytic pyrolysis forms the reaction of propylene/ethylene, and second reaction zone is that methyl alcohol and (or) dimethyl ether and the gas catalysis that contains ethene are converted into propylene/C
4+the reaction of hydrocarbon, wherein the ethylene moiety of the first reaction zone is as the raw material of second reaction zone, the C of second reaction zone
4+hydrocarbon part is as the raw material of the first reaction zone, and arrangement and ethene by two reaction zones transform, and can obtain the propylene of high selectivity.
Catalysis journal, 34 volumes (1 phase), 2013: 209-216 page has been reported " methanol dehydration-C4 cracking olefin hydrocarbon coupled combination technique ", this technique be coupled fluid bed methanol-to-olefins (MTO) and olefins by catalytic cracking (OCC), at utmost increase propylene/ethylene yield.
Above-mentioned patent and open source literature all relate to the fluidized bed reaction system of oxygen-containing compound conversion to produce olefine, and ethene and (or) C
4+hydrocarbon catalytic conversion reaction system, take that to obtain higher propylene/ethylene yield be object, but above-mentioned technique involves two cover independent reaction systems, causes process system very complicated, and fluidized bed reaction system and operation are very complicated, invest highly, reactor need to amplify step by step, amplifies risk high, fixed bed reactors are relatively simple, invest lowly, risk is little, is the better selection of oxygenatedchemicals alkene processed.
Chinese patent CN202844982 discloses the fixed bed reactors of a kind of dimethyl ether and (or) preparing light olefins from methanol, comprise the container with unstrpped gas distributor and lower outlet, at least five modified ZSM-5 type beds are set in container, multidirectional two-tube annular refrigerating gas distributor is set between beds.Reaction feed is dimethyl ether and (or) methyl alcohol, anhydrous or hydrocarbon is as hot diluent media, in conjunction with methanol/dimethyl ether conversion, be that alkene is the fact of strong exothermal reaction, in course of reaction, beds will have very high reaction temperature, thereby cause the irreversible inactivation of ZSM-5 molecular sieve catalyst, be difficult to the stable operation of realization response system, another material facts are, when simple methyl alcohol and (or) dimethyl ether charging, product can be subject to the impact of ZSM-5 special pore structure, causes ethylene/propene yield lower.
Chinese patent CN101460239 discloses the erect-type fixed bed reactors of a kind of oxygenatedchemicals alkene processed, it is characterized in that reactor is provided with 3-8 beds, reactor the first beds is fed to rare oxygenatedchemicals, water and hydrocarbon material, between beds, establish the co-fed nozzle Quench of gas phase dimethyl ether and liquid phase water system, the atomization material that gas-liquid two-phase forms by nozzle mixes uniform to a upper beds discharging, realize the control of next reaction bed temperature.The feed water of this reactor the first beds can reduce charging oxygenatedchemicals and hydrocarbon partial pressure, thereby improves the yield of hydrocarbon and oxygenatedchemicals conversion formation propylene/ethylene.
Chinese patent CN103030504 discloses a kind of production method of producing propylene from methanol/dimethyl ether, adopt fixed bed reactors, pass through water, dimethyl ether contacts with molecular sieve catalyst B in reactor with methyl alcohol to generate and contains propylene, ethene, carbon four, the product of carbon five and carbon six above components thereof, isolate after propylene, again by ethene, carbon four is sent in another reactor and is contacted with molecular sieve catalyst C and further generate propylene with carbon five, object is to solve the lower problem of propene yield in existing methanol-to-olefins technology, but the method still relates to a plurality of reactors, process system is complicated, equipment investment and operating cost are higher.
As can be seen here, improving propylene/ethylene yield in conversion process of oxocompound is emphasis.
Summary of the invention
Object of the present invention is exactly that the fixed bed reactors of a kind of oxygenatedchemicals alkene processed are provided in order to overcome the defect of above-mentioned prior art existence.
Object of the present invention can be achieved through the following technical solutions: the fixed bed reactors of a kind of oxygenatedchemicals alkene processed, these fixed bed reactors are coupling in preparing propylene/ethane from catalytic cracking reaction and oxygenatedchemicals propylene/ethylene processed in a reactor, it is characterized in that, described fixed bed reactors comprise charging aperture, discharging opening and closed container; The charging of described charging aperture is that temperature is the hydrocarbon stream of 400.0～650.0 ℃, or water and hydrocarbon stream; In described closed container, be provided with successively from top to bottom 2～9 beds, between each beds, be provided with intersegmental charging mixed distribution device, wherein between the first paragraph of the superiors, the charging of charging mixed distribution device is water and oxygenatedchemicals logistics, or water, oxygenatedchemicals and hydrocarbon stream, the charging of all the other intersegmental charging mixed distribution devices is water and oxygenatedchemicals;
Temperature is the hydrocarbon stream of 400.0～650.0 ℃, or the first beds that water and hydrocarbon stream enter the superiors through charging aperture carries out olefins by catalytic cracking reaction, reacted material and from water and the oxygenatedchemicals logistics of charging mixed distribution device charging between first paragraph, or water, oxygenatedchemicals and hydrocarbon stream enter next stage beds after mixing, carry out the propylene/ethylene reaction processed of preparing propylene/ethane from catalytic cracking reaction and oxygenatedchemicals simultaneously, reaction products therefrom mixes by beds catalytic reactions at different levels with the charging of each intersegmental charging mixed distribution device successively, until product flows out from discharging opening.
Described hydrocarbon comprises that carbon number is one or more of one to eight alkene and alkane, preferably carbon four, carbon five, carbon six-alkene and-one or more of alkane.
Described oxygenatedchemicals comprises one or both in methyl alcohol, dimethyl ether.
The catalyst loading in described beds is cylindric and/or trifolium-shaped graininess type ZSM 5 molecular sieve.
The physics and chemistry characteristic of the type ZSM 5 molecular sieve loading in described each layer of beds of first beds and all the other can be not identical.
Described fixed bed reactors are axial restraint bed bioreactor or radial fixed-bed reactor.
Described closed container is erect-type or horizontal vessel.
Described intersegmental charging mixed distribution device is gas-liquid two-fluid spray nozzle, adopts manifold and/or many annular spread.
The temperature of each beds is controlled between 400.0-650.0 ℃.
Compared with prior art, the oxygenatedchemicals alkene insulation fix bed reactor processed that the present invention proposes, has following advantage:
1) preparing propylene/ethane from catalytic cracking reaction and oxygenatedchemicals propylene/ethylene processed are coupling in a reactor, have simplified reaction process, also improved the yield of propylene/ethylene.
2) simple structure is easy to amplify, and convenient and flexible operation, invests low.
Accompanying drawing explanation
Fig. 1 is two sections of adiabatic horizontal radial fixed bed reactors;
Fig. 2 is seven sections of erect-type axial restraint bed bioreactors of thermal insulation;
Fig. 3 is nine sections of erect-type axial restraint bed bioreactors of thermal insulation;
Wherein: 1-charging aperture; 2-closed container; 3-the first beds, 5-the second beds, 7-the 3rd beds, 9-the 4th beds, 11-the 5th beds, 13-the 6th beds, 15-the 7th beds, 17-the 8th beds, 19-the 9th beds; Charging mixed distribution device between 4-first paragraph, charging mixed distribution device between 6-second segment, the intersegmental charging mixed distribution device of 8-the 3rd, the intersegmental charging mixed distribution device of 10-the 4th, the intersegmental charging mixed distribution device of 12-the 5th, the intersegmental charging mixed distribution device of 14-the 6th, the intersegmental charging mixed distribution device of 16-the 7th, the intersegmental charging mixed distribution device of 18-the 8th, 20-discharging opening, 21 mass flow pathway a, 23-mass flow pathway b, 22 runner a, 24-runner b.
The specific embodiment
Below in conjunction with the drawings and specific embodiments, the present invention is described in detail.
As two sections of adiabatic horizontal radial fixed bed reactors of Fig. 1, methane, carbon two, carbon four, carbon five, carbon six, carbon seven, carbon eight-alkene and-paraffins mixture material, be heated to be the logistics with 600.0 ℃ of temperature, from charging aperture 1, enter mass flow pathway a21 closed container 2, then radially enter the first beds 3 and carry out catalytic reaction, logistics enters runner a22 after beds 3; Between the first beds 3 and the second beds 5, establish charging mixed distribution device 4 between first paragraph, water, methyl alcohol and dimethyl ether are after intersegmental charging mixed distribution device 4, mix uniform with the discharging of coming from runner, then enter mass flow pathway b23, radially enter subsequently the second beds 5 and carry out catalytic reaction, and this reaction bed temperature is controlled between 400.0-650.0 ℃, product enters runner b24, finally from discharging opening 20, flows out.
As the erect-type axial restraint bed bioreactor of seven sections of thermal insulation of Fig. 2, temperature be 490.0 ℃ water, carbon four, carbon five, carbon six-alkene and-alkane material, through charging aperture 1, enter closed container 2 uniform, then enter the first beds 3 and carry out catalytic reaction; The first beds 3 and the second beds 5 are provided with charging mixed distribution device 4 between first paragraph, water, methyl alcohol, dimethyl ether, carbon four, carbon five, carbon six-alkene and-alkane is after charging mixed distribution device 4 between first paragraph, to the first beds 3 dischargings, mix uniform, then enter the second beds 5 and carry out catalytic reaction, and this reaction bed temperature is controlled between 400.0-650.0 ℃; The second beds 5 and the 3rd beds 7 are provided with charging mixed distribution device 6 between second segment, water, methyl alcohol and dimethyl ether are after charging mixed distribution device 6 between second segment, to the second beds 5 dischargings, mix uniform, then enter the 3rd beds 7 and carry out catalytic reaction, and this reaction bed temperature is controlled between 400.0-650.0 ℃; The 3rd beds 7 and the 4th beds 9 are provided with the 3rd intersegmental charging mixed distribution device 8, water, methyl alcohol and dimethyl ether are after the 3rd intersegmental charging mixed distribution device 8, to the 3rd beds 7 dischargings, mix uniform, then enter the 4th beds 9 and carry out catalytic reaction, and this reaction bed temperature is controlled between 400.0-650.0 ℃; The 4th beds 9 and the 5th beds 11 are provided with the 4th intersegmental charging mixed distribution device 10, water, methyl alcohol and dimethyl ether are after the 4th intersegmental charging mixed distribution device 10, to the 4th beds 9 dischargings, mix uniform, then enter the 5th beds 11 and carry out catalytic reaction, and this reaction bed temperature is controlled between 400.0-650.0 ℃; The 5th beds 11 and the 6th beds 13 are provided with the 5th intersegmental charging mixed distribution device 12, water, methyl alcohol and dimethyl ether are after the 5th intersegmental charging mixed distribution device 12, to the 5th beds 11 dischargings, mix uniform, then enter the 6th beds 13 and carry out catalytic reaction, and this reaction bed temperature is controlled between 400.0-650.0 ℃; The 6th beds 13 and the 7th beds 15 are provided with the 6th intersegmental charging mixed distribution device 14, water, methyl alcohol and dimethyl ether are after the 6th intersegmental charging mixed distribution device 14, to the 6th beds 13 dischargings, mix uniform, then enter the 7th beds 15 and carry out catalytic reaction, and this reaction bed temperature is controlled between 400.0-650.0 ℃, the 7th beds 15 dischargings are flowed out through discharging opening 20.
As the erect-type axial restraint bed bioreactor of nine sections of thermal insulation of Fig. 3, temperature be 470.0 ℃ water, carbon two, carbon four, carbon five, carbon six-alkene and-alkane material, through charging aperture 1, enter closed container 2 uniform, then enter the first beds 3 and carry out catalytic reaction; The first beds 3 and the second beds 5 are provided with charging mixed distribution device 4 between first paragraph, water, methyl alcohol and dimethyl ether are after charging mixed distribution device 4 between first paragraph, to the first beds 3 dischargings, mix uniform, then enter the second beds 5 and carry out catalytic reaction, and this reaction bed temperature is controlled between 400.0-650.0 ℃; The second beds 5 and the 3rd beds 7 are provided with charging mixed distribution device 6 between second segment, water, methyl alcohol and dimethyl ether are after charging mixed distribution device 6 between second segment, to the second beds 5 dischargings, mix uniform, then enter the 3rd beds 7 and carry out catalytic reaction, and this reaction bed temperature is controlled between 400.0-650.0 ℃; The 3rd beds 7 and the 4th beds 9 are provided with the 3rd intersegmental charging mixed distribution device 8, water, methyl alcohol and dimethyl ether are after the 3rd intersegmental charging mixed distribution device 8, to the 3rd beds 7 dischargings, mix uniform, then enter the 4th beds 9 and carry out catalytic reaction, and this reaction bed temperature is controlled between 400.0-650.0 ℃; The 4th beds 9 and the 5th beds 11 are provided with the 4th intersegmental charging mixed distribution device 10, water, methyl alcohol and dimethyl ether are after the 4th intersegmental charging mixed distribution device 10, to the 4th beds 9 dischargings, mix uniform, then enter the 5th beds 11 and carry out catalytic reaction, and this reaction bed temperature is controlled between 400.0-650.0 ℃; The 5th beds 11 and the 6th beds 13 are provided with the 5th intersegmental charging mixed distribution device 12, water, methyl alcohol and dimethyl ether are after the 5th intersegmental charging mixed distribution device 12, to the 5th beds 11 dischargings, mix uniform, then enter the 6th beds 13 and carry out catalytic reaction, and this reaction bed temperature is controlled between 400.0-650.0 ℃; The 6th beds 13 and the 7th beds 15 are provided with the 6th intersegmental charging mixed distribution device 14, water, methyl alcohol and dimethyl ether are after the 6th intersegmental charging mixed distribution device 14, to the 6th beds 13 dischargings, mix uniform, then enter the 7th beds 15 and carry out catalytic reaction, and this reaction bed temperature is controlled between 400.0-650.0 ℃; The 7th beds 15 and the 8th beds 17 are provided with the 7th intersegmental charging mixed distribution device 16, water, methyl alcohol and dimethyl ether are after the 7th intersegmental charging mixed distribution device 16, to the 7th beds 15 dischargings, mix uniform, then enter the 8th beds 17 and carry out catalytic reaction, and this reaction bed temperature is controlled between 400.0-650.0 ℃; The 8th beds 17 and the 9th beds 19 are provided with the 8th intersegmental charging mixed distribution device 18, water, methyl alcohol and dimethyl ether are after the 8th intersegmental charging mixed distribution device 18, to the 8th beds 17 dischargings, mix uniform, then enter the 9th beds 19 and carry out catalytic reaction, and this reaction bed temperature is controlled between 400.0-650.0 ℃, the 9th beds 19 dischargings are flowed out through reactor discharging opening 20.
Claims (10)
1. the fixed bed reactors of an oxygenatedchemicals alkene processed, these fixed bed reactors are coupling in preparing propylene/ethane from catalytic cracking reaction and oxygenatedchemicals propylene/ethylene processed in a reactor, it is characterized in that, described fixed bed reactors comprise charging aperture (1), discharging opening (20) and closed container (2); The charging of described charging aperture (1) is that temperature is the hydrocarbon stream of 400.0～650.0 ℃, or water and hydrocarbon stream; In described closed container, be provided with successively from top to bottom 2～9 beds, between each beds, be provided with intersegmental charging mixed distribution device, wherein between the first paragraph of the superiors, the charging of charging mixed distribution device (4) is water and oxygenatedchemicals logistics, or water, oxygenatedchemicals and hydrocarbon stream, the charging of all the other intersegmental charging mixed distribution devices is water and oxygenatedchemicals;
Temperature is the hydrocarbon stream of 400.0～650.0 ℃, or the first beds that water and hydrocarbon stream enter the superiors through charging aperture (1) carries out olefins by catalytic cracking reaction, reacted material and from water and the oxygenatedchemicals logistics of charging mixed distribution device (4) charging between first paragraph, or water, oxygenatedchemicals and hydrocarbon stream enter next stage beds after mixing, carry out the propylene/ethylene reaction processed of preparing propylene/ethane from catalytic cracking reaction and oxygenatedchemicals simultaneously, reaction products therefrom mixes by beds catalytic reactions at different levels with the charging of each intersegmental charging mixed distribution device successively, until product flows out from discharging opening (20).
2. the fixed bed reactors of a kind of oxygenatedchemicals according to claim 1 alkene processed, is characterized in that, described hydrocarbon comprises that carbon number is one or more of one to eight alkene and alkane.
3. the fixed bed reactors of a kind of oxygenatedchemicals according to claim 1 and 2 alkene processed, is characterized in that, described hydrocarbon comprise carbon four, carbon five, carbon six-alkene and-one or more of alkane.
4. the fixed bed reactors of a kind of oxygenatedchemicals according to claim 1 alkene processed, is characterized in that, described oxygenatedchemicals comprises one or both in methyl alcohol, dimethyl ether.
5. the fixed bed reactors of a kind of oxygenatedchemicals according to claim 1 alkene processed, is characterized in that, the catalyst loading in described beds is cylindric and/or trifolium-shaped graininess type ZSM 5 molecular sieve.
6. the fixed bed reactors of a kind of oxygenatedchemicals according to claim 1 alkene processed, is characterized in that, the physics and chemistry characteristic of the type ZSM 5 molecular sieve loading in described each layer of beds of first beds and all the other can be not identical.
7. the fixed bed reactors of a kind of oxygenatedchemicals according to claim 1 alkene processed, is characterized in that, described fixed bed reactors are axial restraint bed bioreactor or radial fixed-bed reactor.
8. the fixed bed reactors of a kind of oxygenatedchemicals according to claim 1 alkene processed, is characterized in that, described closed container (2) is erect-type or horizontal vessel.
9. the fixed bed reactors of a kind of oxygenatedchemicals according to claim 1 alkene processed, is characterized in that, described intersegmental charging mixed distribution device is gas-liquid two-fluid spray nozzle, adopt manifold and/or many annular spread.
10. the fixed bed reactors of a kind of oxygenatedchemicals according to claim 1 alkene processed, is characterized in that, the temperature of each beds is controlled between 400.0-650.0 ℃.
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112645786A (en) * | 2019-10-12 | 2021-04-13 | 中国石油化工股份有限公司 | Method and system for preparing low-carbon olefin from water-containing raw material |
| CN114225846A (en) * | 2022-01-21 | 2022-03-25 | 中国海洋石油集团有限公司 | Axial-radial flow multi-step feeding fixed bed reactor and preparation method of paraxylene |
| CN114426442A (en) * | 2020-10-15 | 2022-05-03 | 中国石油化工股份有限公司 | Method for preparing low-carbon olefin by using oxygen-containing compound |
| CN115490566A (en) * | 2021-06-18 | 2022-12-20 | 中国石油化工股份有限公司 | Fixed bed reaction system and application thereof, and reaction regeneration method for preparing low-carbon olefin by converting oxygen-containing compound water material |
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| JP2005314339A (en) * | 2004-04-30 | 2005-11-10 | Maruzen Petrochem Co Ltd | Method for production of lower olefin |
| CN103087767A (en) * | 2011-10-28 | 2013-05-08 | 中国石油化工股份有限公司 | Low-carbon olefin production method |
| US20130338418A1 (en) * | 2012-06-14 | 2013-12-19 | Saudi Arabian Oil Company | Direct catalytic cracking of crude oil by a temperature gradient process |
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| JP2005314339A (en) * | 2004-04-30 | 2005-11-10 | Maruzen Petrochem Co Ltd | Method for production of lower olefin |
| CN103087767A (en) * | 2011-10-28 | 2013-05-08 | 中国石油化工股份有限公司 | Low-carbon olefin production method |
| US20130338418A1 (en) * | 2012-06-14 | 2013-12-19 | Saudi Arabian Oil Company | Direct catalytic cracking of crude oil by a temperature gradient process |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112645786A (en) * | 2019-10-12 | 2021-04-13 | 中国石油化工股份有限公司 | Method and system for preparing low-carbon olefin from water-containing raw material |
| CN114426442A (en) * | 2020-10-15 | 2022-05-03 | 中国石油化工股份有限公司 | Method for preparing low-carbon olefin by using oxygen-containing compound |
| CN115490566A (en) * | 2021-06-18 | 2022-12-20 | 中国石油化工股份有限公司 | Fixed bed reaction system and application thereof, and reaction regeneration method for preparing low-carbon olefin by converting oxygen-containing compound water material |
| CN114225846A (en) * | 2022-01-21 | 2022-03-25 | 中国海洋石油集团有限公司 | Axial-radial flow multi-step feeding fixed bed reactor and preparation method of paraxylene |
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