CN102190547B - Improve the method for yield of light olefin products - Google Patents
Improve the method for yield of light olefin products Download PDFInfo
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- CN102190547B CN102190547B CN201010116380.7A CN201010116380A CN102190547B CN 102190547 B CN102190547 B CN 102190547B CN 201010116380 A CN201010116380 A CN 201010116380A CN 102190547 B CN102190547 B CN 102190547B
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/584—Recycling of catalysts
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P30/00—Technologies relating to oil refining and petrochemical industry
- Y02P30/20—Technologies relating to oil refining and petrochemical industry using bio-feedstock
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P30/00—Technologies relating to oil refining and petrochemical industry
- Y02P30/40—Ethylene production
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Abstract
The present invention relates to a kind of method improving yield of light olefin products, mainly solve the problem that in prior art, selectivity of light olefin hydrocarbon is not high.The present invention is by adopting a kind of method improving yield of light olefin products, mainly comprise the following steps: the raw material that (1) comprises methyl alcohol enters the first reaction zone, with comprise silicoaluminophosphamolecular molecular sieve catalyst and contact, generate olefin product I and form decaying catalyst; (2) revivifier that enters at least partially of decaying catalyst regenerates, and the catalyzer regenerated returns to the first reaction zone; (3) catalyst fines running damage in revivifier enters fines collection tank after three cycles are received, then degassing vessel is entered degassed, and enter second reaction zone after mixing with the live catalyst added, with the contact raw comprising carbon more than four hydrocarbon, generate olefin product II, after merging with olefin product I, enter centrifugal station; (4) decaying catalyst of second reaction zone enter revivifier regeneration technical scheme solve the problems referred to above preferably, can be used in the industrial production of light olefin.
Description
Technical field
The present invention relates to a kind of method improving yield of light olefin products.
Technical background
Light olefin, i.e. ethene and propylene, be two kinds of important basic chemical industry raw materials, its demand is in continuous increase.Usually, ethene, propylene are produced by petroleum path, but due to the limited supply of petroleum resources and higher price, produce ethene by petroleum resources, the cost of propylene constantly increases.In recent years, people start to greatly develop the technology that alternative materials transforms ethene processed, propylene.Wherein, the important alternative materials for light olefin production of one class is oxygenatedchemicals, such as alcohols (methyl alcohol, ethanol), ethers (dme, methyl ethyl ether), ester class (methylcarbonate, methyl-formiate) etc., these oxygenatedchemicalss can be transformed by coal, Sweet natural gas, biomass equal energy source.Some oxygenatedchemicals can reach fairly large production, and as methyl alcohol, can be obtained by coal or Sweet natural gas, technique is very ripe, can realize the industrial scale of up to a million tonnes.Due to the popularity in oxygenatedchemicals source, add the economy transforming and generate light olefin technique, so by the technique of oxygen-containing compound conversion to produce olefine (OTO), be particularly subject to increasing attention by the technique of preparing olefin by conversion of methanol (MTO).
Be applied to preparing olefin by conversion of methanol technique to silicoaluminophosphamolecular molecular sieve catalyst in US4499327 patent to study in detail, think that SAPO-34 is the first-selected catalyzer of MTO technique.SAPO-34 catalyzer has very high light olefin selectivity, and activity is also higher, methanol conversion can be made to be less than the degree of 10 seconds in reaction times of light olefin, more even reach in the reaction time range of riser tube.
Technology and reactor that a kind of oxygenate conversion is light olefin is disclosed in US6166282, adopt fast fluidized bed reactor, gas phase is after the lower Mi Xiangfanyingqu of gas speed has reacted, after rising to the fast subregion that internal diameter diminishes rapidly, special gas-solid separation equipment initial gross separation is adopted to go out most entrained catalyst.Due to reaction after product gas and catalyzer sharp separation, effectively prevent the generation of secondary reaction.Through analog calculation, compared with traditional bubbling fluidization bed bioreactor, needed for this fast fluidized bed reactor internal diameter and catalyzer, reserve all greatly reduces.
The multiple riser reaction unit disclosed in CN1723262 with central catalyst return is light olefin technique for oxygenate conversion, this covering device comprises multiple riser reactor, gas solid separation district, multiple offset components etc., each riser reactor has the port of injecting catalyst separately, be pooled to the disengaging zone of setting, catalyzer and gas product are separated.
A kind of method improving yield of light olefins is disclosed in Chinese invention patent 200810043971.9, the method adopts and arranges a second reaction zone on the first top, reaction zone that methanol conversion is low-carbon alkene, and this second reaction zone diameter is greater than the first reaction zone, to increase the residence time of gas product in second reaction zone of the first reaction zone outlet, make unreacted methyl alcohol, the dme generated and carbon more than four hydrocarbon continue reaction, reach the object improving yield of light olefins, the charging that the method also comprises second reaction zone can be through freshening carbon more than four hydrocarbon of separation.Although the method can improve the first trip of low-carbon alkene to a certain extent, but because the first reaction zone catalyzer is out with more carbon distribution, and carbon more than four hydrocarbon pyrolysis needs higher catalyst activity, carbon more than the four hydrocarbon changing effect therefore in the method in second reaction zone is still on the low side.
Therefore, need a kind of novel method, to reach the object being converted into low-carbon alkene making carbon more than four hydrocarbon as far as possible many, finally reach the object improving yield of light olefins and process economy.The present invention solves the problems referred to above targetedly.
Summary of the invention
Technical problem to be solved by this invention is the problem that the selectivity of light olefin hydrocarbon that exists in prior art is not high, provides a kind of method of raising yield of light olefin products newly.The method is used for, in the production of light olefin, having that selectivity of light olefin hydrocarbon is higher, the good advantage of light olefin production process economy.
For solving the problem, the technical solution used in the present invention is as follows: a kind of method improving yield of light olefin products, mainly comprise the following steps: the raw material that (1) comprises methyl alcohol enters the first reaction zone, with comprise silicoaluminophosphamolecular molecular sieve catalyst and contact, generate olefin product I and form decaying catalyst; (2) revivifier that enters at least partially of decaying catalyst regenerates, and the catalyzer regenerated returns to the first reaction zone; (3) catalyst fines running damage in revivifier enters fines collection tank after three cycles are received, then degassing vessel is entered degassed, and enter second reaction zone after mixing with the live catalyst added, with the contact raw comprising carbon more than four hydrocarbon, generate olefin product II, after merging with olefin product I, enter centrifugal station; (4) decaying catalyst of second reaction zone enters revivifier regeneration.
In technique scheme, the first reaction zone, second reaction zone and revivifier are fluidized-bed, and preferred version is: the first reaction zone is fast fluidized bed, and second reaction zone is dense phase fluidized bed, and revivifier is dense phase fluidized bed; Described silicoaluminophosphamolecular molecular sieves is selected from least one in SAPO-5, SAPO-11, SAPO-18, SAPO-20, SAPO-34, SAPO-44, SAPO-56, and preferred version is SAPO-34; Temperature of reaction in described first reaction zone is 400 ~ 500 DEG C, and preferred version is 430 ~ 480 DEG C, and linear gas velocity is 0.8 ~ 2.5 meter per second, and preferred version is 1.0 ~ 1.5 meter per seconds; Temperature of reaction in second reaction zone is 450 ~ 600 DEG C, and preferred version is 500 ~ 550 DEG C, and linear gas velocity is 0.4 ~ 0.9 meter per second, and preferred version is 0.6 ~ 0.8 meter per second; Described fine powder is the granules of catalyst that median size is less than 30 microns, and the median size of described live catalyst is 50 ~ 100 microns; By adding live catalyst in degassing vessel, the catalyzer median size in second reaction zone is kept to be 40 ~ 80 microns; Described three are threaded to second reaction zone scope inner catalyst handling equipment all needs insulation; Decaying catalyst in described second reaction zone is entering revivifier regeneration after water vapour stripping; The top gas outlet of described second reaction zone arranges three and revolves recovery of catalyst fines, delivers to fines collection tank.
The preparation method of silicoaluminophosphamolecular molecular sieve of the present invention is: first prepare molecular sieve precursor, is 0.03 ~ 0.6R: (Si0.01 ~ 0.98: Al0.01 ~ 0.6: P0.01 ~ 0.6): 2 ~ 500H by mol ratio
2o, wherein R represents template, and constitutive material mixed solution, obtains at a certain temperature after the crystallization of certain hour; Again, after molecular sieve precursor, phosphorus source, silicon source, aluminium source, organic formwork agent, water etc. being mixed according to certain ratio, at 110 ~ 260 DEG C, hydrothermal crystallizing, after at least 0.1 hour, finally obtains SAPO molecular sieve.
Mixed with a certain proportion of binding agent by the molecular sieve of preparation, after the operation steps such as spraying dry, roasting, obtain final SAPO catalyzer, the weight percentage of binding agent in molecular sieve is generally between 10 ~ 90%.
Two reaction zones is provided with in the method for the invention, first reaction zone is relatively independent, for preparing olefin by conversion of methanol, second reaction zone, for transforming carbon more than four hydrocarbon or transforming unreacted methyl alcohol or dme etc., reaches the object improving feed stock conversion and yield of light olefins.Wherein, second reaction zone is dense phase fluidized bed, ensures the enough reaction times, and maximized conversion carbon more than four hydrocarbon is low-carbon alkene, and its parameter such as material level, temperature of reaction can independently control.And the present inventor finds through research, regenerator outlet runs the catalyst fines damaged and has higher catalytic activity, if mix a certain proportion of live catalyst, adjusts the size distribution of mixed catalyst, can high efficiency conversion carbon more than four high-carbon hydrocarbon.When the catalyst fines in system runs up to a certain degree, a part can be drawn off in segmentation holding tank and recycle.In second reaction zone, the catalyzer of inactivation returns revivifier regeneration, has so just shared a revivifier with the first reaction zone.Therefore, adopt method of the present invention, the object improving selectivity of light olefin hydrocarbon can be reached.
Adopt technical scheme of the present invention: the first reaction zone, second reaction zone and revivifier are fluidized-bed; Described silicoaluminophosphamolecular molecular sieves is selected from least one in SAPO-5, SAPO-11, SAPO-18, SAPO-20, SAPO-34, SAPO-44, SAPO-56; Temperature of reaction in described first reaction zone is 400 ~ 500 DEG C, and linear gas velocity is 0.8 ~ 2.5 meter per second; Temperature of reaction in second reaction zone is 450 ~ 600 DEG C, and linear gas velocity is 0.4 ~ 0.9 meter per second; Described fine powder is the granules of catalyst that median size is less than 30 microns, and the median size of described live catalyst is 50 ~ 100 microns; By adding live catalyst in degassing vessel, the catalyzer median size in second reaction zone is kept to be 40 ~ 80 microns; Described three are threaded to second reaction zone scope inner catalyst handling equipment all needs insulation; Decaying catalyst in described second reaction zone is entering revivifier regeneration after water vapour stripping; The top gas outlet of described second reaction zone arranges three and revolves recovery of catalyst fines, and deliver to fines collection tank, yield of light olefins can reach 92.43% weight, achieves good technique effect.
Accompanying drawing explanation
Fig. 1 is the schematic flow sheet of the method for the invention.
In Fig. 1,1 is the first reaction zone bottom feed; 2 is the first reaction zone; 3 is the first reaction zone products export pipeline; 4 is the line of pipes that in the first reaction zone, decaying catalyst enters revivifier; 5 is regenerating medium source line; 6 is revivifier; 7 is flue gas and catalyst fines outlet line; 8 is three to revolve; 9 is fines collection tank; 10 is fines collection pot bottom discharging pipeline; 11 is three revolve exhanst gas outlet pipeline; 12 is degassing vessel; 13 is second reaction zone; 14 is second reaction zone bottom feed; 15 enter the line of pipes of revivifier for second reaction zone decaying catalyst; 16 is second reaction zone top gas outlet line; 17 enter the catalyst transport pipeline of second reaction zone for degassing vessel; 18 enter the catalyst transport pipeline of the first reaction zone for revivifier regenerated catalyst; 19 enter degassed line of pipes for fines collection tank catalyzer; 20 fine powders received for second reaction zone top exit three cycle enter the pipeline of fines collection tank; 21 is the pipeline adding live catalyst to degassing vessel.
Raw material enters in the first reaction zone 2 through feeding line 1, contacts with molecular sieve catalyst, and reaction generates the product stream I containing light olefin, and decaying catalyst enters revivifier regeneration from reclaimable catalyst inclined tube 4.Catalyzer after having regenerated returns to the first reaction zone from regenerated catalyst inclined tube 18.Fines collection tank 9 is entered after the catalyst fines running damage in revivifier revolves 8 recovery through three, then degassing vessel 12 is entered degassed, and enter second reaction zone 13 after mixing with the live catalyst added, with the contact raw comprising carbon more than four hydrocarbon, generate olefin product II, after merging with olefin product I, enter centrifugal station; The decaying catalyst of second reaction zone 13 enters revivifier regeneration from pipeline 15.
Below by embodiment, the invention will be further elaborated, but be not limited only to the present embodiment.
Embodiment
[embodiment 1]
In reaction unit as shown in Figure 1, the first reaction zone is fast fluidized bed, and medial temperature is 480 DEG C, and linear gas velocity is 1.5 meter per seconds; Second reaction zone is dense phase fluidized bed, and medial temperature is 550 DEG C, and linear gas velocity is 0.8 meter per second; Revivifier is dense phase fluidized bed, and medial temperature is 660 DEG C.First reaction zone bottom feed is pure methyl alcohol, and charging is 2 kgs/hr, and catalyzer is SAPO-34, wherein SiO in molecular sieve
2: Al
2o
3: P
2o
5=0.1: 1: 1, in catalyzer, binder content is 60%.Second reaction zone bottom feed is mixed c 4, and the fine powder that C 4 olefin content 87%, three revolves collection after measured median size is 20 microns, and the median size of live catalyst is 80 microns; By adding live catalyst in degassing vessel, the catalyzer median size in second reaction zone is kept to be 60 microns, three are threaded to second reaction zone scope inner catalyst handling equipment is all incubated, decaying catalyst in second reaction zone is entering revivifier regeneration after water vapour stripping, second reaction zone top gas outlet arranges three and revolves recovery of catalyst fines, after deliver to fines collection tank, second reaction zone products export and the first reaction zone products export merge and enter separate part.Keep the stability of catalyst flow control, reactor outlet product adopts online gas chromatographic analysis, and yield of light olefins reaches 90.46% weight.
[embodiment 2]
According to the condition described in embodiment 1, the first reaction zone medial temperature is 500 DEG C, and linear gas velocity is 2.5 meter per seconds; Second reaction zone medial temperature is 600 DEG C, and linear gas velocity is 0.9 meter per second.Keep the stability of catalyst flow control, reactor outlet product adopts online gas chromatographic analysis, and yield of light olefins reaches 89.47% weight.
[embodiment 3]
According to the condition described in embodiment 1, the first reaction zone medial temperature is 400 DEG C, and linear gas velocity is 0.8 meter per second; Second reaction zone medial temperature is 450 DEG C, and linear gas velocity is 0.4 meter per second.Keep the stability of catalyst flow control, reactor outlet product adopts online gas chromatographic analysis, and yield of light olefins reaches 84.26% weight.
[embodiment 4]
According to the condition described in embodiment 1, the first reaction zone medial temperature is 430 DEG C, and linear gas velocity is 1.0 meter per seconds; Second reaction zone medial temperature is 500 DEG C, and linear gas velocity is 0.6 meter per second.Keep the stability of catalyst flow control, reactor outlet product adopts online gas chromatographic analysis, and yield of light olefins reaches 87.87% weight.
[embodiment 5]
According to the condition described in embodiment 1, three fine powders revolving collection after measured median size are 18 microns, the median size of live catalyst is 50 microns, the catalyzer median size in second reaction zone is kept to be 40 microns, keep the stability of catalyst flow control, reactor outlet product adopts online gas chromatographic analysis, and yield of light olefins reaches 88.72% weight.
[embodiment 6]
According to the condition described in embodiment 1, three fine powders revolving collection after measured median size are 28 microns, the median size of live catalyst is 100 microns, the catalyzer median size in second reaction zone is kept to be 80 microns, keep the stability of catalyst flow control, reactor outlet product adopts online gas chromatographic analysis, and yield of light olefins reaches 91.46% weight.
[embodiment 7]
According to the condition described in embodiment 1, just change the type of catalyzer Middle molecule sieve, experimental result is in table 1.
Table 1
| Parameter | Molecular sieve type | Yield of light olefins, % (weight) |
| Embodiment 9 | SAPO-20 | 81.54 |
| Embodiment 10 | SAPO-18 | 88.11 |
| Embodiment 11 | SAPO-56 | 70.34 |
| Embodiment 12 | SAPO-34+SAPO-18 (weight ratio is 2: 1) | 89.04 |
[embodiment 8]
According to the condition described in embodiment 1, second reaction zone bottom feed is the mixture of mixed c 4 and unreacted methyl alcohol and dme, olefin(e) centent wherein in mixed c 4 is 87%, the weight ratio of mixed c 4 and methyl alcohol and dme is 4: 1, keep the stability of catalyst flow control, reactor outlet product adopts online gas chromatographic analysis, and yield of light olefins reaches 92.43% weight.
[embodiment 9]
According to the condition described in embodiment 1, SiO in molecular sieve
2: Al
2o
3: P
2o
5=0.2: 1: 1, in catalyzer, binder content is 70%., light olefin carbon base absorption rate is 88.02% (weight).
[comparative example 1]
According to the condition described in embodiment 1, do not establish second reaction zone, run damage catalyst fines and only reclaim and be not used, low-carbon alkene carbon base absorption rate is 79.5% weight.
Obviously, adopt method of the present invention, the object improving selectivity of light olefin hydrocarbon can be reached, there is larger technical superiority, can be used in the industrial production of light olefin.
Claims (8)
1. improve a method for yield of light olefin products, mainly comprise the following steps:
(1) raw material comprising methyl alcohol enters the first reaction zone, and comprises silicoaluminophosphamolecular molecular sieve catalyst and contacts, and generates olefin product I and forms decaying catalyst;
(2) revivifier that enters at least partially of decaying catalyst regenerates, and the catalyzer regenerated returns to the first reaction zone;
(3) catalyst fines running damage in revivifier enters fines collection tank after three cycles are received, then degassing vessel is entered degassed, and enter second reaction zone after mixing with the live catalyst added, with the contact raw comprising carbon more than four hydrocarbon, generate olefin product II, after merging with olefin product I, enter centrifugal station;
(4) decaying catalyst of second reaction zone enters revivifier regeneration;
Wherein, by adding live catalyst in degassing vessel, the catalyzer median size in second reaction zone is kept to be 40 ~ 80 microns; Second reaction zone top gas outlet arranges three and revolves recovery of catalyst fines, delivers to fines collection tank.
2. improve the method for yield of light olefin products according to claim 1, it is characterized in that described first reaction zone, second reaction zone and revivifier are fluidized-bed; Described silicoaluminophosphamolecular molecular sieves is selected from least one in SAPO-5, SAPO-11, SAPO-18, SAPO-20, SAPO-34, SAPO-44, SAPO-56.
3. improve the method for yield of light olefin products according to claim 2, it is characterized in that described first reaction zone is fast fluidized bed, second reaction zone is dense phase fluidized bed, and revivifier is dense phase fluidized bed; Described molecular screening is from SAPO-34.
4. improve the method for yield of light olefin products according to claim 1, it is characterized in that the temperature of reaction in described first reaction zone is 400 ~ 500 DEG C, linear gas velocity is 0.8 ~ 2.5 meter per second; Temperature of reaction in second reaction zone is 450 ~ 600 DEG C, and linear gas velocity is 0.4 ~ 0.9 meter per second.
5. improve the method for yield of light olefin products according to claim 4, it is characterized in that the temperature of reaction in described first reaction zone is 430 ~ 480 DEG C, linear gas velocity is 1.0 ~ 1.5 meter per seconds; Temperature of reaction in second reaction zone is 500 ~ 550 DEG C, and linear gas velocity is 0.6 ~ 0.8 meter per second.
6. improve the method for yield of light olefin products according to claim 1, it is characterized in that described fine powder is the granules of catalyst that median size is less than 30 microns, the median size of described live catalyst is 50 ~ 100 microns.
7. improve the method for yield of light olefin products according to claim 1, it is characterized in that described three be threaded to second reaction zone scope inner catalyst handling equipment all need insulation.
8. improve the method for yield of light olefin products according to claim 1, it is characterized in that the decaying catalyst in described second reaction zone is entering revivifier regeneration after water vapour stripping.
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|---|---|---|---|---|
| CN1345361A (en) * | 1999-02-17 | 2002-04-17 | 埃克森化学专利公司 | Catalytic conversion of oxygenates to olefins |
| CN101260015A (en) * | 2008-04-24 | 2008-09-10 | 中国石油化工股份有限公司 | Method for preparing low-carbon olefins from oxygen-containing compound |
| CN101270023A (en) * | 2008-04-11 | 2008-09-24 | 中国石油化工股份有限公司 | Method for improving selectivity of light olefin hydrocarbon |
| CN101332434A (en) * | 2008-07-08 | 2008-12-31 | 中国石油化工股份有限公司 | Processing method of low carbon olefin hydrocarbon reactor escaping lost catalyst produced by methanol or dimethyl ether |
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Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1345361A (en) * | 1999-02-17 | 2002-04-17 | 埃克森化学专利公司 | Catalytic conversion of oxygenates to olefins |
| CN101270023A (en) * | 2008-04-11 | 2008-09-24 | 中国石油化工股份有限公司 | Method for improving selectivity of light olefin hydrocarbon |
| CN101260015A (en) * | 2008-04-24 | 2008-09-10 | 中国石油化工股份有限公司 | Method for preparing low-carbon olefins from oxygen-containing compound |
| CN101332434A (en) * | 2008-07-08 | 2008-12-31 | 中国石油化工股份有限公司 | Processing method of low carbon olefin hydrocarbon reactor escaping lost catalyst produced by methanol or dimethyl ether |
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