CN102351629A - Method for producing propylene and high-octane gasoline from methanol - Google Patents
Method for producing propylene and high-octane gasoline from methanol Download PDFInfo
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- CN102351629A CN102351629A CN2011102425498A CN201110242549A CN102351629A CN 102351629 A CN102351629 A CN 102351629A CN 2011102425498 A CN2011102425498 A CN 2011102425498A CN 201110242549 A CN201110242549 A CN 201110242549A CN 102351629 A CN102351629 A CN 102351629A
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Abstract
The invention discloses a method for producing propylene and high-octane gasoline from methanol, which comprises steps as follows: methanol and water pass through an olefin preparation reactor and enters a deethanizing column; the separated C3+ material enters a depropanizing column, the separated C3 material enters a rectifying column, and the separated C4+ material enters an etherification reactor; the rectifying column separates out propane and propylene; the C4+ material enters the etherification reactor to react with methanol, the generated etherified gasoline is discharged out of the device, the unreacted C4+ material and C2 and C2- components are mixed to recoincide for dehydrocyclization; and the materials after reaction are separated to obtain dry gas, liquefied petroleum gas and a liquid material containing rich aromatic hydrocarbons. On the premise of obtaining high propylene yield, the byproduct containing rich olefins are subjected to etherification and coincidence dehydrocyclization reaction to coproduce the high-octane gasoline blended component; and the invention has the advantages of obvious economic benefit, simple overall process and low investment.
Description
Technical field
The present invention relates to a kind of method of utilizing methanol production propylene and stop bracket gasoline blend component.Especially when methyl alcohol generated propylene through catalyst reaction, utilization other reaction product except that propylene carries out etherificate and the process that generates the stop bracket gasoline blend component is reacted in superimposed dehydrocyclization.
Background technology
Propylene is one of most important basic organic that is only second to by ethene, and its maximum purposes is to produce Vestolen PP 7052, accounts for 52%.According to CMAI, global in recent years propylene demand year rate of rise has substantially exceeded ethene, and the major cause that the propylene supply increases fast is because due to the polyacrylic demand rapid growth of verivate.Because the China's oil resource is in short supply, utilize petroleum path to produce propylene and satisfied not needs far away, the propylene demand gap is very big, has had influence on the development of downstream chemical industry.Coal resources in China is abundant relatively, utilizes abundant coal to produce low-carbon alkene to China organic chemical industry sustainable development, and power supply safety has great strategic importance.Coal system alkene technology is raw material with coal; Through technological processs such as gasification, synthesising gas systeming carbinol, methanol-to-olefins; Be methanol-to-olefins technology (MTO) and preparing propylene from methanol technological (MTP), these two core technologies that technology is a coal system alkene at present wherein for representative.
The methanol-to-olefins technology can be widened propylene feedstocks channel, adjustment raw material mix, reduces the dependence to petroleum resources.At present, the industrial demonstration unit that this technology is checked and approved through country has one, the MTO of group of Shenhua project, and the provincial project of checking and approving has two, is respectively the MTP project of Shenhua Ningxia Coal Industry Group and Datang derived energy chemical ltd.Various places have 28 (incomplete statistics) according to statistics in the project of planning, and the market temperature is very high.The technology that the methanol-to-olefins technology possesses industrialized condition has the MTO technology of UOP/Hydro company, the Chinese Academy of Sciences's big fluidization thing DMTO technology and Oil of Shanghai Petrochemical Company research institute SMTO technology.The sophisticated MTP technology that Lurgi is arranged of preparing propylene from methanol technical development, the circulating fluidized bed preparing propylene from methanol FMTP technology of Tsing-Hua University.Wherein Lurgi company, the Dalian Chemistry and Physics Institute of Chinese Academy of Sciences industry demonstration unit are driven, and Tsing-Hua University is just at the building industry testing apparatus.Under the level of soaring oil prices, MTO and MTP technology have the low economic advantages of cost than steam cracking and catalytic cracking raising the output system propylene technology.
The patent that with methyl alcohol is the oxygen-containing organic compound of the representative process aspect of producing ethene and propylene is a lot.
Chinese patent 96115333.4 has been introduced and has a kind ofly been produced ethene by methyl alcohol or dme; The method of low-carbon alkenes such as propylene adopts the SAPO-34 sieve catalyst, on the ciculation fluidized reaction unit of dense bed, carries out the continuous circulation of this reacting middle catalyst and reacts and the regenerated method;
Chinese patent 99815451.2 has been introduced through the reaction-regeneration that on the micro-spherical catalyst based on the SAPO-34 zeolite, in fluidized-bed reactor-regenerator system, takes place to continue, and methanol conversion one-tenth is had the 93-100% degree of conversion and greater than 90% C optionally
2-C
4The method of low-molecular olefine;
Chinese patent 01144188.7 is a kind of process method and system thereof by dme or preparing low carbon olefin hydrocarbon with methanol, and this process using silicoaluminophosphamolecular molecular sieves (SAPO-34) utilizes the ultrashort contact reactor of gas-solid cocurrent flow descending formula fluidized-bed as catalyzer.Through process method and the system that uses this invention, reduced the generation of by product alkane, reduce the difficulty of follow-up separation process, and then increased the output of product low-carbon alkene.
Chinese patent 200710064232.3 provide a kind of with methyl alcohol or/and dme is the method that raw material is produced low-carbon alkene; The method is characterized in that with methyl alcohol that or/and dme is divided into three reaction zone feeds by a certain percentage the ratio through regulating three reaction zone feeds and the reaction conditions of each reaction zone obtain required olefin product and distribute.
Chinese patent 200710037232.4 relates to the method for a kind of methyl alcohol or dimethyl ether conversion producing light olefins, mainly solves the make charcoal problem of the bad control of degree, the bad assurance of catalyst in reactor average activity level of revivifier in the prior art.
Chinese patent 200710037234.3 relates to a kind of method that in methyl alcohol or dimethyl ether conversion process, improves selectivity of light olefin, mainly solves the lower problem of selectivity of light olefin in the existing methanol-to-olefins technology.
Chinese patent 200480022527.9 provides and has been used for from comprising ethane; Ethene; Propylene; Dme, and one or more the initial flow in propane, acetylene, methylacetylene, propadiene, methane, hydrogen, carbon monoxide, carbonic acid gas and the C4+ component goes out the novel high effective separation method and the system of separation of polymeric level ethene and propylene in the materials flow.
The separation method that China 200610017775.5 discloses a kind of converting methanol to prepare low carbon olefin (DMTO) gas, the characteristics that constitute to DMTO gas are improved the flow process after four sections compressions in the conventional front-end deethanization separation process.According to the present invention, setting adds the hydrogen-oxygen conversion between five sections compressions and deethanizing column return tank, removes the oxygen that produces in acetylene and the reaction regeneration process; The cooled material of condensation is through the deethanizing column return tank; Liquid phase refluxes as deethanizing column, and gas phase gets into deep cooling demethanizing system, after material cools off through condensation; The preceding dehydrogenation system of loaded down with trivial details ice chest need be set, directly get into high pressure demethanizer.Adopt the present invention to separate DMTO gas and can obtain the ethylene recovery rate more than 99.5%.
To sum up patent is said; What relate generally to is that methanol conversion is catalyst research, reactor drum improvement, the optimization of process conditions that improves olefins yield and the improvement of product separation process of low-carbon alkene; Prior art is with the further cracking of these components; Be converted into propylene, to improve propylene selectivity and productive rate.Do not have and carry out the integrated patent of method of utilizing about utilization other reaction product except that propylene.
Summary of the invention
Technical problem to be solved by this invention provides a kind of method of utilizing methanol production propylene and stop bracket gasoline; Can provide improved and generate the integrated flow of propylene, particularly optimize integrated work flow and scheme that methyl alcohol generates the comprehensive utilization of by product behind the propylene by methyl alcohol.
In order to realize the object of the invention, a kind of method idiographic flow of methanol production propylene and stop bracket gasoline that utilizes of the present invention is:
(1), methyl alcohol and water charge ratio are 1.0～5.0 (weight); Beds system olefine reaction through the system olefin hydrocarbon reactor; The reactor drum pattern is fixed-bed reactor, and catalyzer is the bar shaped catalyst of active ingredient for the ZSM-5 molecular sieve, 400～600 ℃ of temperature of reaction; Reaction pressure 0.1～2.0MPa, methyl alcohol weight space velocity are 0.5～5.0h
-1(weight) gets into deethanizing column through the reaction product behind the system olefin hydrocarbon reactor;
(2), get into deethanizing column from the reaction product of step (1) and separate, isolate material and be C2 and less than C2 component and C3
+Material, wherein C3
+Material goes out deethanizing column and gets into depropanizing tower;
(3), from the C3 of step (2)
+Material gets into depropanizing tower, isolates C3 material and C4
+Material, wherein isolated C3 material gets into rectifying tower, isolated C4
+Material gets into the etherification reaction device;
(4), get into rectifying tower, isolate propane and propylene, these two kinds of materials go out device respectively from the C3 material of step (3); Purified propylene after the rectifying can be adjusted as required, for example can reach the polymerization-grade standard, and propane weight purity can reach 90～99%;
(5), from the C4 of step (3)
+Material gets into etherification reaction device and methyl alcohol reaction, and the etherified gasoline that reaction generates goes out device, has neither part nor lot in the C4 of reaction
+Material gets into superimposed dehydrocyclization device again; Etherification reaction temperature is 60～80 ℃, and reaction velocity is 3.0～5.0h
-1(weight), reaction pressure are 0.50～1.0MPa;
(6), from the C4 that has neither part nor lot in reaction in the step (5)
+Material and from step (2) material C2 and be mixed into superimposed dehydrocyclization reaction unit less than the C2 component carries out superimposed dehydrocyclization reaction, and reacting rear material is separated, and obtains dry gas, LPG liquefied petroleum gas and is rich in the liquid material of aromatic hydrocarbons; Superimposed dehydrocyclization temperature of reaction is that 350～450 ℃, reaction velocity are 0.5～2.0h
-1(weight), reaction pressure are 0.1～0.5 MPa.
It is 50～70% product liquid that reaction can obtain total aromaticity content, and propane content is 70～85% (weight) in the LPG liquefied petroleum gas.
Described system olefin hydrocarbon apparatus catalyzer is to be the catalyzer of active ingredient with the ZSM-5 molecular sieve, and this ZSM-5 belongs to high silica alumina ratio series.
Production propylene of the present invention and stop bracket gasoline flow process, its etherification reaction is identical with conventional etherification reaction, and the structure of reactor pattern is identical with catalyzer with the catalyzer also etherification reaction device reaction type formula with routine.Concrete, described etherification reaction device, its reactor drum can be fixed-bed reactor, catalyzer can be Zeo-karb, molecular sieve, solid super-strong acid or the sulfuric acid catalyst of the etherification reaction of routine.
Concrete, described superimposed dehydrocyclization device, its reactor drum is fixed-bed reactor, catalyzer is that zeolite molecular sieve is the bar shaped catalyst in active site.More specifically, this catalyzer is to be the commercial catalyst of active ingredient with low silica-alumina ratio ZSM-5 molecular sieve, the Sinopec catalyst Co.
SKP-2Catalyzer.
Further concrete, in the above-mentioned steps (5), the alfin ratio of reaction raw materials methyl alcohol/iso-butylene (mol/mol) is the best with 1.0～1.1.
The described C2 material of this patent, C2 component are meant that carbon atom number is 2 hydrocarbon component.
The described C3 of this patent
+Material, C3
+Component is meant that carbon atom number is more than or equal to 3 hydrocarbon component.
The described C4 of this patent
+Material, C4
+Component is meant that carbon atom number is more than or equal to 4 hydrocarbon component.
The above-mentioned steps flow process, the LPG liquefied petroleum gas mixing of materials that wherein generates in isolating propane material and the step (6) in the step (4) can be used as motor liquified gas.What wherein superimposed dehydrocyclization generated in reaction generation etherified gasoline and the step (6) in the step (5) is rich in the arene liquid material through mix, can be used as the stop bracket gasoline blend component.
The main products that the present invention is based on methanol conversion and be propylene technology is a propylene; While by-product fuel gas, LPG liquefied petroleum gas and petroleum naphtha (C5～C7); Wherein be rich in ethene in the fuel gas; Be rich in C 4 olefin (especially iso-butylene is main) in the LPG liquefied petroleum gas, petroleum naphtha is rich in alkene (especially isopentene and dissident's alkene are main).This part by product that is rich in alkene can utilize machinery to process, and produces the stop bracket gasoline blend component to improve its added value.The machinery that relates generally to is that fuel gas advances superimposed dehydrocyclization device and generates the component that height contains aromatic hydrocarbons; LPG liquefied petroleum gas and petroleum naphtha get into ether-based device and the methyl alcohol reaction generates etherified gasoline; LPG liquefied petroleum gas gets into superimposed dehydrocyclization device and generates the component that height contains aromatic hydrocarbons equally after the etherificate, can be used as the stop bracket gasoline blend component after these three kinds of resultant of reaction material mix.
This patent is through the improvement of reaction process; Each device relating to all has under the situation of maturing appts,, on guaranteed basis on the product yield; Several kinds of products of existing apparatus are comprised that olefin component is reprocessed in dry gas, the liquefied gas, form a new technical process.When obtaining high productivity of propylene, the by product that is rich in alkene can coproduction stop bracket gasoline blend component through etherificate, superimposed dehydrocyclization reaction, remarkable in economical benefits, whole flow process simply, less investment.
Description of drawings
Fig. 1 is the schematic flow sheet that utilizes methanol production propylene and stop bracket gasoline blend component.
Among the figure, 1, methyl alcohol, 2, the preparing propylene from methanol device, 3, deethanizing column, 4 ,≤the C2 component, 5, C3
+Component, 6, depropanizing tower, 7, the C3 rectifying tower, 8, C4
+Component, 9, the etherification reaction device, 10, C4 after the etherificate
+Component, 11, superimposed dehydrocyclization device, 12, propylene, 13, propane, 14, dry gas, 15, motor liquified gas, 16, the stop bracket gasoline blend component.
Embodiment
Embodiment 1
As shown in Figure 1, raw material 1 reacts with water access to plant 2, and processing condition are 400～600 ℃ of temperature of reaction, and reaction pressure 0.1～2.0MPa, methyl alcohol weight space velocity are 0.5～5.0h
-1(weight); Catalysts is an active constituent catalyst for high silica alumina ratio ZSM-5; Reacting rear material gets into 3; Here the material 4 formed of C2 and lighter gaseous fraction is transferred to from cat head and is got into follow-up device 11 and carry out superimposed dehydrocyclization reaction, and temperature of reaction is that 350～450 ℃, reaction velocity are 0.5～2.0h
-1(weight), reaction pressure is 0.1～0.5 Mpa, and catalysts is the Sinopec catalyst Co.
SKP-2Catalyzer, principal reaction material are ethene; Be admitted to device 6 from installing the material 5 that comes out 3 bottoms; The C3 component is left access to plant 7 from cat head, and the propylene of recovered overhead polymerization-grade, propane are then incorporated follow-up material 15 pipe networks into.Comprise C4 hydro carbons and other heavier components from installing the material 8 that comes out 6 bottoms, this component and methyl alcohol access to plant 9 together carry out etherification reaction, and etherification reaction temperature is 60～80 ℃, and reaction velocity is 3.0～5.0h
-1(weight), reaction pressure are 0.50～1.0Mpa, and catalyzer can be Zeo-karb, molecular sieve, solid super-strong acid or the sulfuric acid catalyst of the etherification reaction of routine.The etherification reaction of isomeric olefine and methyl alcohol generates etherified gasoline in the material; Part unreacted material 10 accesss to plant 11 carry out superimposed dehydrocyclization reaction, and the high aromatic hydrocarbon content product liquid that gasoline and superimposed dehydrocyclization device come out behind the etherification reaction mixes back component material 16.Material carries out the material 14 that superimposed dehydrocyclization reaction back produces at device 11 and gets into the fuel gas pipe networks, device 11 reactions produce LPG liquefied petroleum gas mix back materials 15 as motor liquified gas with device 7 isolating materials 13.
Behind preparing propylene from methanol series of optimum reaction process, reaction product is a dry gas, propylene; Motor liquified gas, the stop bracket gasoline blend component, preparing propylene from methanol reaction back by product is fully used; Added value is higher; Remarkable in economical benefits of the present invention, whole flow process is simple, less investment, is the integrated work flow of ideal preparing propylene from methanol.
Table 1: the difference (raw material is a methyl alcohol) of conventional MTP flow process and this integrated flow
Claims (8)
1. method of utilizing methanol production propylene and stop bracket gasoline is characterised in that idiographic flow is:
(1), methyl alcohol and water charge ratio are 1.0～5.0 (weight); Beds system olefine reaction through the system olefin hydrocarbon reactor; The reactor drum pattern is fixed-bed reactor, and catalyzer is the bar shaped catalyst of active ingredient for the ZSM-5 molecular sieve, 400～600 ℃ of temperature of reaction; Reaction pressure 0.1～2.0MPa, methyl alcohol weight space velocity are 0.5～5.0h
-1(weight) gets into deethanizing column through the reaction product behind the system olefin hydrocarbon reactor;
(2), get into deethanizing column from the reaction product of step (1) and separate, isolate material and be C2 and less than C2 component and C3
+Material, wherein C3
+Material goes out deethanizing column and gets into depropanizing tower;
(3), from the C3 of step (2)
+Material gets into depropanizing tower, isolates C3 material and C4
+Material, wherein isolated C3 material gets into rectifying tower, isolated C4
+Material gets into the etherification reaction device;
(4), get into rectifying tower, isolate propane and propylene, these two kinds of materials go out device respectively from the C3 material of step (3);
(5), from the C4 of step (3)
+Material gets into etherification reaction device and methyl alcohol reaction, and the etherified gasoline that reaction generates goes out device, has neither part nor lot in the C4 of reaction
+Material gets into superimposed dehydrocyclization device again; Etherification reaction temperature is 60～80 ℃, and reaction velocity is 3.0～5.0h
-1(weight), reaction pressure are 0.50～1.0Mpa;
(6), from the C4 that has neither part nor lot in reaction in the step (5)
+Material and from step (2) material C2 and be mixed into superimposed dehydrocyclization reaction unit less than the C2 component carries out superimposed dehydrocyclization reaction, and reacting rear material is separated, and obtains dry gas, LPG liquefied petroleum gas and is rich in the liquid material of aromatic hydrocarbons; Superimposed dehydrocyclization temperature of reaction is that 350～450 ℃, reaction velocity are 0.5～2.0h
-1(weight), reaction pressure are 0.1～0.5 Mpa.
2. according to the said a kind of method of utilizing methanol production propylene and stop bracket gasoline of claim 1, it is characterized in that: described system olefin hydrocarbon apparatus, its reactor drum are fixed-bed reactor, and catalyzer is for being the high silica alumina ratio catalyzer of active ingredient with ZSM-5.
3. according to the said a kind of method of utilizing methanol production propylene and stop bracket gasoline of claim 1; It is characterized in that: described etherification reaction device; Its reactor drum is fixed-bed reactor, and catalyzer is Zeo-karb, molecular sieve, solid super-strong acid or the sulfuric acid catalyst of the etherification reaction of routine.
4. according to the said a kind of method of utilizing methanol production propylene and stop bracket gasoline of claim 3, it is characterized in that: etherification reaction temperature is 60～80 ℃, and reaction velocity is 3.0～5.0h
-1(weight).
5. according to the said a kind of method of utilizing methanol production propylene and stop bracket gasoline of claim 1, it is characterized in that: the alfin ratio of reaction raw materials methyl alcohol/iso-butylene (mol/mol) is 1.0～1.1.
6. according to the said a kind of method of utilizing methanol production propylene and stop bracket gasoline of claim 1; It is characterized in that; It is characterized in that: the reactor drum of superimposed dehydrocyclization device is fixed-bed reactor, and catalyzer is that zeolite molecular sieve is the metal-modified bar shaped catalyst of process in active site.
7. according to the said a kind of method of utilizing methanol production propylene and stop bracket gasoline of claim 6, it is characterized in that, it is characterized in that: superimposed dehydrocyclization temperature of reaction is that 350～450 ℃, reaction velocity are 0.5～2.0h
-1(weight).
8. according to the said a kind of method of utilizing methanol production propylene and stop bracket gasoline of claim 6; It is characterized in that: the metallic element method of modifying is for adopting saturated or supersaturation dipping solubility salt, will adopting sedimentary method to deposit metal on the molecular sieve; Through roasting metal is fixed on the molecular sieve again after the drying, reaches modification molecular sieve.
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103242884A (en) * | 2013-05-20 | 2013-08-14 | 易高环保能源研究院有限公司 | Process for preparing high-octane high-cleanness gasoline with methanol by using multi-element catalysis method |
| CN105254462A (en) * | 2015-11-03 | 2016-01-20 | 中国石油大学(华东) | Process for producing olefin from methanol and for co-producing gasoline and aromatic hydrocarbon |
| CN108404983A (en) * | 2018-03-23 | 2018-08-17 | 华东师范大学 | A kind of preparation and its application of ordered mesoporous phenolic resin Polymer-supported silver catalyst |
| CN110157480A (en) * | 2019-05-10 | 2019-08-23 | 国家能源投资集团有限责任公司 | The method and its application that the increment of process of preparing propylene from coal-based methanol high-carbon by-product utilizes |
| CN114907178A (en) * | 2021-02-07 | 2022-08-16 | 中国石油天然气股份有限公司 | Method for producing C2-C3 olefin and high-octane gasoline blending component by using C4-C6 hydrocarbon as raw material |
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| US4826507A (en) * | 1987-12-08 | 1989-05-02 | Mobil Oil Corporation | Integrated etherification and oxygenates to gasoline process |
| CN101333461A (en) * | 2008-03-25 | 2008-12-31 | 北京惠尔三吉绿色化学科技有限公司 | Method for producing cleaning fuel oil form petroleum cracking dry gas and C4 component |
| WO2011006594A1 (en) * | 2009-07-14 | 2011-01-20 | Lurgi Gmbh | Method and apparatus for producing synthetic fuels |
-
2011
- 2011-08-23 CN CN2011102425498A patent/CN102351629B/en active Active
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4826507A (en) * | 1987-12-08 | 1989-05-02 | Mobil Oil Corporation | Integrated etherification and oxygenates to gasoline process |
| CN101333461A (en) * | 2008-03-25 | 2008-12-31 | 北京惠尔三吉绿色化学科技有限公司 | Method for producing cleaning fuel oil form petroleum cracking dry gas and C4 component |
| WO2011006594A1 (en) * | 2009-07-14 | 2011-01-20 | Lurgi Gmbh | Method and apparatus for producing synthetic fuels |
Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103242884A (en) * | 2013-05-20 | 2013-08-14 | 易高环保能源研究院有限公司 | Process for preparing high-octane high-cleanness gasoline with methanol by using multi-element catalysis method |
| CN105254462A (en) * | 2015-11-03 | 2016-01-20 | 中国石油大学(华东) | Process for producing olefin from methanol and for co-producing gasoline and aromatic hydrocarbon |
| CN108404983A (en) * | 2018-03-23 | 2018-08-17 | 华东师范大学 | A kind of preparation and its application of ordered mesoporous phenolic resin Polymer-supported silver catalyst |
| CN108404983B (en) * | 2018-03-23 | 2020-08-04 | 华东师范大学 | Preparation and application of ordered mesoporous phenolic resin polymer supported silver catalyst |
| CN110157480A (en) * | 2019-05-10 | 2019-08-23 | 国家能源投资集团有限责任公司 | The method and its application that the increment of process of preparing propylene from coal-based methanol high-carbon by-product utilizes |
| CN110157480B (en) * | 2019-05-10 | 2021-04-20 | 国家能源投资集团有限责任公司 | Value-added utilization method of high-carbon byproduct in process of preparing propylene from coal-based methanol and application of value-added utilization method |
| CN114907178A (en) * | 2021-02-07 | 2022-08-16 | 中国石油天然气股份有限公司 | Method for producing C2-C3 olefin and high-octane gasoline blending component by using C4-C6 hydrocarbon as raw material |
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|---|---|
| CN102351629B (en) | 2013-11-20 |
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