CN101417914A - Method for preparing propylene from methanol using hydrocarbons as part material - Google Patents
Method for preparing propylene from methanol using hydrocarbons as part material Download PDFInfo
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- CN101417914A CN101417914A CNA2007101764050A CN200710176405A CN101417914A CN 101417914 A CN101417914 A CN 101417914A CN A2007101764050 A CNA2007101764050 A CN A2007101764050A CN 200710176405 A CN200710176405 A CN 200710176405A CN 101417914 A CN101417914 A CN 101417914A
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Abstract
The invention relates to a preparation method of propylene, in particular to a method for preparing light olefins, which takes methanol, carbon 4 and the hydrocarbons above carbon 4 are taken as raw material. In the process cracking ethylene and/or dimethyl ether to prepare propylene, part of from carbon 4 to carbon 18 alkane and olefin are added as feedings, and the scission reaction of hydrocarbon which absorbs heat is used for reducing the lot quantity of heat of reaction released from the cracking process of ethylene and/or dimethyl ether, thereby inhibiting the heat effect of the MTO reaction, raising the stability of the reaction system, allowing the operation easier, prolonging the service of catalytic agent, saving energy and reducing cost.
Description
Technical field
The present invention relates to the preparation method of propylene, being specifically related to methyl alcohol and carbon four and above hydro carbons is the method for feedstock production propylene.
Background technology
Propylene is a kind of important organopolysiloxane oil chemical industry basic raw material that is only second to ethene, is mainly used in the production of polypropylene (PP).Along with maintaining sustained and rapid growth of polypropylene demand, more and more big to the demand of propylene, bigger pressure is being born in traditional propylene source.Simultaneously, along with the minimizing day by day of petroleum resources, more aggravated the present situation of propylene short supply.Therefore, be that raw material is produced propylene technology via methyl alcohol or dme and more and more received concern both domestic and external with coal or Sweet natural gas.
In the eighties in 20th century, it is the research of low-carbon alkene that U.S. Mobil oil company has just begun methanol conversion.What make a breakthrough is the MTO technology that American UOP company and Norway Norsk Hydro company develop jointly, and this technology is used the SAPO-34 molecular sieve catalyst, has higher yield of ethene.What preparing propylene from methanol technology was representative is the MTP technology of strange (Lurgi) company in German Shandong exploitation, and the catalyzer that this technology uses German southern chemical company to provide has high propene yield.
Process of preparing low carbon olefinic hydrocarbon with methanol is a strong thermopositive reaction, because of the reaction very exothermic causes the catalyst carbon deposit deactivation rate very fast.Therefore, the MTO technology is generally all used fluidized-bed reactor, to realize the cyclic regeneration of catalyzer; MTP technology is used changeable regenerated fixed-bed reactor.But because the problem of reaction heat adds a large amount of water as thinner or thermal barrier in the raw material of being everlasting when actually operating.Gasification, the condensation therein of a large amount of water increased the energy consumption in the technological process greatly, and reduced the space-time yield of target product.
Produce many patents aspect the propylene in methanol conversion, for example US5714662A1, US5191141A1, US5744680A1, US6534692, US6166282A etc., catalyst system therefor is all based on the SAPO-34 molecular sieve, adopt fluidized-bed reactor, with water content is that 20% methyl alcohol is raw material, and ethylene selectivity is higher in the low-carbon alkene.The operating temperature range of reactive system is 350 ℃～525 ℃, and by the regulation and control of processing condition, ethylene/propene can be 1.5～0.64 variations in the low-carbon alkene.When stable operation, the weight percentage of ethene, propylene, carbon tetraene is respectively in the hydrocarbon product: 40%, 38%, 11%.
It is the method for raw material production propylene with methyl alcohol that European patent EP 0448000 has been introduced a kind of, this method adopts fixed-bed reactor, the weight ratio 0.1～1.5 of water and methyl alcohol in the raw material, catalyst system therefor is the Si-Al molecular sieve of Zn, Cd modification, for reducing the reaction heat of reactive system, raw material is earlier by pre-reactor dehydration, and what enter main reactor is the mixture of methyl alcohol, dme and water.The reactive system temperature range is 280 ℃～570 ℃, and system pressure 10kPa～90kPa generates ethene, propylene in the low-carbon alkene, and the weight percentage of carbon tetraene in the generation hydrocarbon product is no less than 5%, 35%, 30% respectively.
Chinese patent CN1084431A is catalyzer with the modified zsm-5 zeolite, is the feedstock production low-carbon alkene with methyl alcohol or dme, adopts 2～n cracking reactor to react-regenerate switching successively, to realize continuous operation.Because emit a large amount of reaction heat in the reaction process, the ratio of methyl alcohol and water is 3:7 in the charging, by the heat effect that is used for reducing in the reaction process that makes of Macrodilution agent water.
Produce in the catalytic cracking process of ethene and refinery at cracking petroleum hydrocarbon vapor, the above hydro carbons of C4 and C4 (based on C4 alkene) is main by product, and how effectively utilizing this part resource is the important topic that ethylene plant and refinery face jointly.If with the part charging of this part C4 and above hydro carbons as preparing propylene from methanol, then can utilize this part hydrocarbon cracking to need the characteristics of a large amount of heats, effectively reduce the heat effect of reacting in the preparing propylene from methanol process, help improving the stability of reactive system, make to be reflected at easier operation on the engineering; Simultaneously and since C4 and above hydro carbons at high temperature the cracked primary product also be based on propylene, therefore, in the preparing propylene from methanol process, add the yield that portion C 4 and above hydro carbons also help to improve target product.
Summary of the invention
The technical problem to be solved in the present invention is:
At the deficiencies in the prior art, the purpose of this invention is to provide a kind of is that the methyl alcohol of part material prepares cyclopropene method with the hydro carbons, produce in the process of propylene at methyl alcohol and/or dme cracking, add part carbon four and carbon four above hydro carbons as common charging, utilize the hydrocarbon cracking that absorbs heat to react and reduce a large amount of reaction heat that discharged in methyl alcohol and/or the dme cracking process.
Technical scheme of the present invention is:
A kind of is that the methyl alcohol of part material prepares cyclopropene method with the hydro carbons, comprising:
Use two kinds of raw materials, first kind of raw material is: at least a in methyl alcohol and the dme; Can be single methyl alcohol, also can be single dme, can also be the mixture of methyl alcohol and dme.
Second kind of raw material is at least a in following: carbon four to carbon octadecane hydrocarbon, carbon four to carbon octadecylene hydrocarbon; Can be a kind of above-mentioned alkane or a kind of above-mentioned alkene, also can be the mixture of above-mentioned alkane or the mixture of above-mentioned alkene, can also be the mixture of above-mentioned alkane and alkene, and alkene can be monoolefine, also can be polyene hydrocarbon.Contain olefin fraction more than five as various C-4-fractions, C5 fraction, the carbon of producing ethene, propylene unit or plant catalytic cracking unit from steam cracking, with and composition thereof.
The ratio of two kinds of raw materials is, described first kind of raw material be in moles of methanol, with the ratio of second kind of feed molar number is:
First kind of raw material: second kind of raw material=1:0.05～10
Wherein, in first kind of raw material per 1 mole of dme in 2 mole, of methanol;
Promptly the mole number of first kind of raw material is amounting to into the mole number of methyl alcohol, and the mole number of second kind of raw material is in the actual mole number of carbon four to carbon octadecane hydrocarbon, alkene.
Prepare at methyl alcohol under the effect of propylene catalyst, above-mentioned two kinds of raw materials are reacted in reactor, generate propylene.Usually also comprise some by products.
Inventive point of the present invention is carbon four and above hydro carbons are produced the part charging that propylene reacts (MTP) as methyl alcohol and/or dme, because carbon four and above hydro carbons are under hot conditions, the cracked primary product also is based on propylene on the MTP catalyzer, therefore, can be when not influencing or improving propene yield, play the reduction reaction heat effect, improve the effect of reactive system stability, make to be reflected at easier operation on the engineering.
In the present invention,, the heat effect of reaction is effectively extenuated, help the catalyzer prolongation in work-ing life owing to add carbon four and above hydro carbons.Because carbon four and above hydro carbons are during as common charging, the heat effect of entire reaction significantly reduces, make the reaction bed temperature in the reaction process be tending towards even, in the time of independent methyl alcohol and/or dme can occurring and be reaction raw materials, the too high phenomenon of reaction occurrence positions temperature in the catalyzer micropore, so the coking deactivation speed of catalyzer slows down, catalyst life is longer than originally.
In the present invention, can use any catalyzer that can realize methyl alcohol and/or dimethyl ether production propylene, or multiplely have a described function mixture of catalysts.Hybrid mode comprises that two or more catalyzer combines or the simple physics fusion by tackiness agent or auxiliary agent.The MTP catalyzer is a known technology, and used catalyzer but is not got rid of the use that other has function catalyzer of the present invention for being the catalyzer of main active ingredient with the ZSM-5 molecular sieve in the embodiment of the invention.
In the described reactor, reaction pressure is a normal pressure, and temperature of reaction is 300 ℃～650 ℃, and mass space velocity is 0.1h
-1～10h
-1
With before described catalyzer contacts, described second kind of raw material mixes with described first kind of raw material at described first kind of raw material.The charging form that is reactor can be selected different modes, as:
Described first kind of raw material adds described reactor with after described second kind of raw material directly mixes;
Also can described second kind of raw material be injected described first kind of material feeding at described reactor inlet place;
Described first kind of raw material is in the charging of reactor inlet place, with described second kind of raw material injecting reactor before the reactor catalyst bed.
Add diluent gas in the described reaction system, described diluent gas is to be selected from least a in following: nitrogen, helium, argon gas, hydrogen, methane, ethane, propane, butane, carbon monoxide, carbonic acid gas, water vapour.
In molar ratio, diluent gas: raw material=0～1:1
Above-mentioned raw materials calculates with the mole number sum of first kind of raw material and second kind of raw material.
Be that raw material can be with charging behind the inert gas dilution, also can be without diluent gas, diluent gas is not participated in reaction.When industrial application, described diluent gas can recycle.The separation of diluent gas and Recycle design can adopt the known technology of industrial routine.
The present invention is raw materials used for having added methyl alcohol and/or the dme parallel feeding of part carbon four to carbon 18 hydro carbons, owing to add carbon four to carbon 18 hydro carbons, the heat that methyl alcohol and/or dme cracking are discharged is compared during with independent charging and is effectively extenuated, and therefore can or reduce the consumption of the water of thermal barrier effect in reaction process.
Usually, described reactor is: at least a in fixed-bed reactor, fluidized-bed reactor and the moving-burden bed reactor.Promptly when using a reactor, can be fixed-bed reactor, fluidized-bed reactor or moving-burden bed reactor also; When using many reactors, can use identical reactor, also can use different reactors.
Because the present invention has prolonged the work-ing life of catalyzer, therefore reaction of the present invention can realize on the fixed-bed reactor that MTP technology is used always, also can on fluidized-bed reactor, carry out, also not get rid of simultaneously and use moving-bed etc. other can realize the reactor of process of the present invention.
When concrete operations, first kind of raw material can obtain with the methyl alcohol pre-reaction: earlier methyl alcohol is sent into pre-reactor, wherein the part methanol conversion becomes dme, and the product that will contain methyl alcohol and dme again adds described reactor as described first kind of raw material with described second kind of raw material.Also be that dme in the raw material is directly by methanol conversion.
Usually, to prepare propylene catalyst be at least a in following to described methyl alcohol: have tart natural molecule sieve, have the tart synthesis of molecular sieve.Promptly can have a tart natural molecule sieve, or have a tart synthesis of molecular sieve with a kind of with a kind of, also can be with the mixture of above-mentioned molecular sieve.
Further preferred, described methyl alcohol prepares propylene catalyst and is selected from least a in following: X type molecular sieve, Y zeolite, ZSM type molecular sieve, SAPO type molecular sieve, the molecular sieve modified product of X type, Y zeolite modified product, the molecular sieve modified product of ZSM type, the molecular sieve modified product of SAPO type.Promptly can be a kind of in X type molecular sieve or its modified product, Y zeolite or its modified product, ZSM type molecular sieve or its modified product, SAPO type molecular sieve or its modified product, also can be the mixture of multiple above-mentioned zeolite product.
Especially, described methyl alcohol prepares propylene catalyst and is selected from least a in following: type ZSM 5 molecular sieve, ZSM-5 type molecule modified product.
It can be that independent a kind of catalyzer is by the tackiness agent moulding that described methyl alcohol prepares propylene catalyst.Used tackiness agent is known routine techniques, and shaping of catalyst also is a known technology.
Described methyl alcohol prepares propylene catalyst: multiple catalyzer with different catalytic performances combines by tackiness agent becomes mixed catalyst or multiple catalyzer with different catalytic performances becomes mixed catalyst by the physics fusion.
According to general catalyzer common practise, described methyl alcohol prepares propylene catalyst can add auxiliary agent in preparation process, and described auxiliary agent comprises at least a in various known binding agents, pore-forming material, dispersion agent, the lubricant.
At least a during described second kind of raw material is preferably following: carbon four to carbon ten alkane, carbon four to carbon ten alkene; At least a in further preferably following: carbon four to carbon six alkane, carbon four to C 6 olefin.
Described first kind of raw material be in moles of methanol, with the preferred proportion of second kind of feed molar number is:
First kind of raw material: second kind of raw material=1:0.1～2.
Further preferred proportion is first kind of raw material: second kind of raw material=1:0.1～0.5.
The invention has the beneficial effects as follows:
The present invention is by preparing to carbon octadecane hydrocarbon, alkene carbon four the common charging of low-carbon alkene as methyl alcohol and/or dme cracking, the hydrocarbon cracking reaction that a large amount of reaction heat of being discharged in methyl alcohol and/or the dme cracking process are absorbed heat absorbs, thereby the heat effect that has suppressed the MTO reaction, thereby reactive system stability, processing ease have been improved; Reaction bed temperature is tending towards evenly, and the coking deactivation speed of catalyzer will be slowed down, and catalyst life is prolonged; Reduce the consumption of thinner, conserve energy; Cost is descended.
Embodiment
Further describe the present invention below in conjunction with embodiment.Scope of the present invention is not subjected to the restriction of these embodiment, and scope of the present invention proposes in claims.
Embodiment 1 Preparation of catalysts
The delivery number is that 3.6 water glass 156g is dissolved in the 50g water.Other gets 1g content is 99% Al
2(SO
4)
318H
2O is that 98% the vitriol oil and 75ml water mix with 15g content then.Under vigorous stirring, two kinds of solution are mixed, and to add 50g content be 10% TPAOH template, continue to stir and make into the homogeneous gel shape.Change gelatigenous object over to stainless steel crystallization device, airtight, in 180 ℃ of crystallization 50 hours.After crystallization was finished, product was cooled off rapidly, and inclining mother liquor, the centrifugation throw out, and with the pure water washing for several times, be 8～9 until the pH of solution value, then the gained crystallisate was descended dry 12 hours at 120 ℃, 5 hours removed template methods of 550 ℃ of following roastings obtain the ZSM-5 molecular sieve.
The gained ZSM-5 molecular sieve NH of 1mol/L
4After the exchange of Cl solution, got Hydrogen ZSM-5 molecular sieve in 4 hours in 550 ℃ of following roastings.With this molecular sieve and Al
2O
3Binding agent is pressed the mixed of 2:1, and extrusion moulding on banded extruder promptly gets to test and uses catalyzer.
Embodiment 2
On the fixed-bed reactor of continuous flow, the catalyzer 3ml that filling embodiment 1 is prepared.Under normal pressure, blowing air, flow velocity 50ml/min in 500 ℃ of following calcined catalysts 2 hours, switches to N then
2Purged 0.5 hour.With N
2Be carrier gas, flow velocity 50ml/min, methyl alcohol and C 4 olefin are raw material, and mol ratio is methyl alcohol: C 4 olefin=1:0.167, mass space velocity are 3h
-1, temperature of reaction is 490 ℃.Table 1 is that the raw material of C 4 olefin is formed.Table 2 is the preparing propylene from methanol reaction result of C 4 olefin during as the part charging.
Comparative Examples 1
Adopt catalyzer and the experiment condition identical with embodiment 2, raw material is a methyl alcohol, and temperature of reaction is 490 ℃, and experimental result sees Table 2.
Table 1 C 4 olefin weight percent is formed
| Form | 1-butylene | Suitable-2-butylene | Instead-2-butylene | Iso-butylene |
| Content, % | 22.3 | 43.1 | 19.8 | 14.8 |
Table 2 C 4 olefin is as common charging methanol to olefins reaction result
| Embodiment 2 | Comparative Examples 1 | |
| Charging | CH 3OH+C4 | CH 3OH |
| The outer temperature of reaction tubes, ℃ | 490 | 490 |
| The reaction bed temperature, ℃ | 493 | 496 |
| The one way activity cycle, h | 38 | 24 |
| Product is formed | wt％ | wt％ |
| Methyl alcohol+dme | 0 | 0 |
| C1+C2+C3 | 6.32 | 5.68 |
| C2＝ | 15.16 | 14.65 |
| C3＝ | 36.24 | 34.57 |
| C4 | 16.18 | 18.62 |
| C5+ | 12.83 | 14.92 |
| Aromatic hydrocarbons | 9.068.31 |
| COx | 4.213.25 |
Embodiment 3
Adopt catalyzer, raw material, the experiment condition identical with embodiment 2, the experimental result when temperature of reaction is respectively 450 ℃, 560 ℃ sees Table 3.
Table 3 C 4 olefin is as common charging methanol to olefins reaction result
| Temperature, ℃ | 450 | 560 |
| Product is formed | wt％ | wt％ |
| Methyl alcohol+dme | 0 | 0 |
| C1+C2+C3 | 1.58 | 8.21 |
| C2＝ | 18.62 | 12.32 |
| C3＝ | 32.95 | 36.01 |
| C4 | 20.18 | 14.52 |
| The C5+ hydrocarbon | 12.53 | 10.83 |
| Aromatic hydrocarbons | 11.32 | 12.13 |
| COx | 2.82 | 5.98 |
Embodiment 4
Adopt catalyzer and the experiment condition identical with embodiment 2, raw materials used be methyl alcohol and the mixture of octene just, and mol ratio is methyl alcohol: octene=1:0.1 just, experimental result sees Table 4.
Embodiment 5
Adopt catalyzer and the experiment condition identical with embodiment 2, raw materials used be methyl alcohol and the mixture of laurylene just, and mol ratio is methyl alcohol: laurylene=1:0.067 just, experimental result sees Table 4.
Table 4 C8 alkene and C12 alkene are as common charging preparing propylene from methanol reaction result
| Embodiment 4 | Implement 5 | |
| Charging | CH 3OH+C8＝ | CH 3OH+C12＝ |
| Product is formed | wt％ | wt％ |
| Methyl alcohol+dme | 0 | 0 |
| C1+C2+C3，％ | 5.43 | 4.18 |
| C2＝ | 13.86 | 13.11 |
| C3＝ | 34.12 | 33.62 |
| C4 | 19.32 | 20.06 |
| The C5+ hydrocarbon | 13.21 | 12.68 |
| Aromatic hydrocarbons | 9.5 | 10.99 |
| COx | 4.56 | 5.36 |
Embodiment 6
Adopt catalyzer and the raw material identical, with carrier gas N with embodiment 2
2Replace with water, the input speed of water is 4g/ml, and other reaction conditions is constant, and experimental result sees Table 5.
Table 5 C 4 olefin is as common charging methanol to olefins reaction result
| Product is formed | wt％ |
| Methyl alcohol+dme | 0 |
| C1+C2+C3 | 6.01 |
| C2＝ | 15.86 |
| C3＝ | 36.82 |
| C4 | 15.48 |
| C5+ | 11.95 |
| Aromatic hydrocarbons | 10.02 |
| COx | 3.86 |
Claims (10)
1 one kinds is that the methyl alcohol of part material prepares cyclopropene method with the hydro carbons, it is characterized in that:
Use two kinds of raw materials, first kind of raw material is: at least a in methyl alcohol and the dme;
Second kind of raw material is at least a in following: carbon four to carbon octadecane hydrocarbon, carbon four to carbon octadecylene hydrocarbon;
Described first kind of raw material be in moles of methanol, with the ratio of second kind of feed molar number is:
First kind of raw material: second kind of raw material=1:0.05～10
Wherein, in first kind of raw material per 1 mole of dme in 2 mole, of methanol;
Prepare at methyl alcohol under the effect of propylene catalyst, above-mentioned two kinds of raw materials are reacted in reactor, generate propylene.
2 according to claim 1 be that the methyl alcohol of part material prepares cyclopropene method with the hydro carbons, it is characterized in that:
In the described reactor, reaction pressure is a normal pressure, and temperature of reaction is 300 ℃～650 ℃, and mass space velocity is 0.1h
-1～10h
-1
With before described catalyzer contacts, described second kind of raw material mixes with described first kind of raw material at described first kind of raw material.
3 according to claim 1 be that the methyl alcohol of part material prepares cyclopropene method with the hydro carbons, it is characterized in that:
Add diluent gas in the described reaction system, described diluent gas is to be selected from least a in following: nitrogen, helium, argon gas, hydrogen, methane, ethane, propane, butane, carbon monoxide, carbonic acid gas, water vapour;
In molar ratio, diluent gas: raw material=0～1:1
Above-mentioned raw materials calculates with the mole number sum of first kind of raw material and second kind of raw material.
4 according to claim 1 be that the methyl alcohol of part material prepares cyclopropene method with the hydro carbons, it is characterized in that:
Described reactor is: at least a in fixed-bed reactor, fluidized-bed reactor and the moving-burden bed reactor.
5 according to claim 1 be that the methyl alcohol of part material prepares cyclopropene method with the hydro carbons, it is characterized in that:
Earlier methyl alcohol is sent into pre-reactor, wherein the part methanol conversion becomes dme, and the product that will contain methyl alcohol and dme again adds described reactor as described first kind of raw material with described second kind of raw material.
6 according to claim 1 be that the methyl alcohol of part material prepares cyclopropene method with the hydro carbons, it is characterized in that:
It is at least a in following that described methyl alcohol prepares propylene catalyst: have tart natural molecule sieve, have the tart synthesis of molecular sieve.
7 according to claim 6 be that the methyl alcohol of part material prepares cyclopropene method with the hydro carbons, it is characterized in that:
Described methyl alcohol prepares propylene catalyst and is selected from least a in following: X type molecular sieve, Y zeolite, ZSM type molecular sieve, SAPO type molecular sieve, the molecular sieve modified product of X type, Y zeolite modified product, the molecular sieve modified product of ZSM type, the molecular sieve modified product of SAPO type.
Preferably: described methyl alcohol prepares propylene catalyst and is selected from least a in following: type ZSM 5 molecular sieve, ZSM-5 type molecule modified product.
8 according to claim 6 be that the methyl alcohol of part material prepares cyclopropene method with the hydro carbons, it is characterized in that:
Described methyl alcohol prepares propylene catalyst and add auxiliary agent in preparation process, and described auxiliary agent comprises at least a in various known binding agents, pore-forming material, dispersion agent, the lubricant.
9 described according to one of claim 1 to 9 be that the methyl alcohol of part material prepares cyclopropene method with the hydro carbons, it is characterized in that:
Described second kind of raw material is at least a in following: carbon four to carbon ten alkane, carbon four to carbon ten alkene.Preferably: carbon four to carbon six alkane, carbon four to C 6 olefin.
10 according to claim 1 be that the methyl alcohol of part material prepares cyclopropene method with the hydro carbons, it is characterized in that:
First kind of raw material: second kind of raw material=1:0.1～2.
Preferably, first kind of raw material: second kind of raw material=1:0.1～0.5.
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| CN101928598A (en) * | 2010-09-28 | 2010-12-29 | 上海应用技术学院 | Method and system for producing gasoline and propylene by integrating heavy oil catalytic cracking with oxygen-containing compound conversion |
| CN102372574A (en) * | 2010-08-27 | 2012-03-14 | 中国石油化工股份有限公司 | Method for preparing propylene by cracking C4 olefin added with methanol and/or dimethyl ether |
| CN103130603A (en) * | 2011-11-30 | 2013-06-05 | 中国科学院大连化学物理研究所 | Method for preparing low-carbon alkene by promoting conversion of pentane |
| CN103130605A (en) * | 2011-11-30 | 2013-06-05 | 中国科学院大连化学物理研究所 | Method for preparing low-carbon olefin by promoting conversion of butane |
| CN106831288A (en) * | 2017-03-06 | 2017-06-13 | 江苏天诺新材料科技股份有限公司 | The MTP methods of mixed alcohol side entry feed |
| CN106866329A (en) * | 2017-01-22 | 2017-06-20 | 江苏天诺新材料科技股份有限公司 | The preparation method of low-carbon alkene |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6455749B1 (en) * | 1997-10-03 | 2002-09-24 | Exxonmobil Chemical Patents, Inc. | Method for increasing light olefin yield by conversion of a heavy hydrocarbon fraction of a product to light olefins |
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| CN102372574A (en) * | 2010-08-27 | 2012-03-14 | 中国石油化工股份有限公司 | Method for preparing propylene by cracking C4 olefin added with methanol and/or dimethyl ether |
| CN101928598A (en) * | 2010-09-28 | 2010-12-29 | 上海应用技术学院 | Method and system for producing gasoline and propylene by integrating heavy oil catalytic cracking with oxygen-containing compound conversion |
| CN103130603A (en) * | 2011-11-30 | 2013-06-05 | 中国科学院大连化学物理研究所 | Method for preparing low-carbon alkene by promoting conversion of pentane |
| CN103130605A (en) * | 2011-11-30 | 2013-06-05 | 中国科学院大连化学物理研究所 | Method for preparing low-carbon olefin by promoting conversion of butane |
| CN103130603B (en) * | 2011-11-30 | 2016-03-02 | 中国科学院大连化学物理研究所 | A kind of method promoting conversion of pentane producing light olefins |
| CN103130605B (en) * | 2011-11-30 | 2016-03-02 | 中国科学院大连化学物理研究所 | A kind of method promoting conversion of butane producing light olefins |
| CN107964414A (en) * | 2016-10-19 | 2018-04-27 | 深圳市新路田科技有限公司 | A kind of method and system of coupling between methanol liquefied petroleum gas lightweight low-coagulation diesel oil |
| CN106866329A (en) * | 2017-01-22 | 2017-06-20 | 江苏天诺新材料科技股份有限公司 | The preparation method of low-carbon alkene |
| CN106831288A (en) * | 2017-03-06 | 2017-06-13 | 江苏天诺新材料科技股份有限公司 | The MTP methods of mixed alcohol side entry feed |
| CN106831288B (en) * | 2017-03-06 | 2019-07-26 | 江苏国瓷天诺新材料科技股份有限公司 | The MTP method of mixed alcohol side entry feed |
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