CN100537713C - A kind of catalysis conversion method of producing more propylene - Google Patents
A kind of catalysis conversion method of producing more propylene Download PDFInfo
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- CN100537713C CN100537713C CNB2005100898504A CN200510089850A CN100537713C CN 100537713 C CN100537713 C CN 100537713C CN B2005100898504 A CNB2005100898504 A CN B2005100898504A CN 200510089850 A CN200510089850 A CN 200510089850A CN 100537713 C CN100537713 C CN 100537713C
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Abstract
A kind of catalysis conversion method of producing more propylene, riser reactor is co-axial each other first reaction zone, second reaction zone, optional outlet area and level pipe from bottom to up successively, level pipe links to each other with settling vessel, and first reaction zone is connected the catalyst inlet pipe respectively with the second reaction zone bottom; The unstripped gas of preheating is injected a reactor that comprises two reaction zones, enter first reaction zone with the catalyst mix of heat, under 250～450 ℃ temperature of reaction, carry out building-up reactions, and then and the catalyst mix of another part heat enter second reaction zone, under 450～650 ℃ of temperature of reaction, carry out cracking and dehydrogenation reaction, after reaction was finished, separated product, reclaimable catalyst entered and recycle after revivifier burns.Adopt the light hydrocarbons that method provided by the invention can be less with the economic worth after isolating propylene through gas separation system to transform the higher propylene of generation economic worth.
Description
Technical field
The present invention relates to a kind of under the situation that does not have hydrogen the catalysis conversion method of petroleum hydrocarbon, more particularly, be a kind of catalysis conversion method that utilizes light hydrocarbons to produce propylene.
Background technology
Catalytic cracking is one of most important technological process of petroleum refining industry.Conventional catalytic cracking technology mostly adopts isodiametric single riser reactor and reaction-regeneration system flow process.In the riser tube reaction-regeneration system, the stock oil of preheating enters riser reactor through the feed nozzle system, contacts, vaporizes and react with high temperature catalyst (title regenerated catalyst) from revivifier.Constantly generate coke in the reaction process and be deposited on catalyst surface and the active centre on, make activity of such catalysts descend the selectivity variation.For this reason, coked catalyst (title reclaimable catalyst) in time separated with reaction oil gas and enter revivifier carry out coke burning regeneration, and then recycle.Reaction oil gas then enters separation system and isolates light-end products, in the raw material after primary first-order equation unconverted heavy oil can enter once more and carry out cracking reaction in the riser reactor.The general industry riser reactor is about 30～40 meters, about 4～5 meter per seconds of reactor inlet rate of flow of fluid, and along with the carrying out of cracking reaction, the minimizing of product molecular-weight average, about 15～18 meter per seconds of fluid outlet flow velocity, about 1～3 second of total reaction time.
Though the bed reactor that the early stage catalytic cracking process of riser reactor adopts is much superior, but also there is the improved place of many needs, mainly show: (1) riser tube exit catalyst performance sharply descends, and second half section cracking reaction condition is more abominable; (2) for some secondary reaction, the reaction times is too short, thereby has suppressed some secondary reactions useful to quality product; (3) just near piston flow, still there is air-teturning mixed phenomenon from flow pattern in riser reactor; (4) reactor internal reaction condition is more single and fixing, difficultly adapts to current catalytically cracked stock and forms changeablely, and market requirement frequent variations causes complicated situation that products distribution and product property requirement are also changed at any time.For this reason, people constantly improve riser reactor, overcoming these drawbacks, such as:
A kind of riser reactor is disclosed among the CN1237477A, this reactor vertically be followed successively by co-axial each other pre lift zone, first reaction zone, enlarged-diameter from bottom to up second reaction zone, reduced outlet area, at the outlet area end one level pipe is arranged.It is different with the processing condition of second reaction zone that this reactor both can optionally have been controlled first reaction zone, can make the stock oil of different performance carry out the segmentation cracking again, obtains required purpose product.Producing Trimethylmethane and being rich in the catalysis conversion method of isoparaffin gasoline based on above-mentioned new texture riser reactor disclosed among the CN1232069A, this method is that the stock oil after the preheating is injected a reducing reactor that comprises two reaction zones, contact with the cracking catalyst of heat, 530～620 ℃ of first reaction zone temperatures, 0.5～2.0 second reaction times; 460～530 ℃ of second reaction zone temperatures, 2～30 seconds reaction times, reaction product isolated, reclaimable catalyst enters through stripping and recycles after revivifier burns.Adopt that Trimethylmethane content is 20～40 heavy % in the liquefied gas that this method produces, the isoparaffin content during gasoline family forms is 30～45 heavy %, and olefin(e) centent is reduced to below the 30 heavy %, and its research octane number (RON) is 90～93, and motor-method octane number is 80～84.
Propylene is important Organic Chemicals, and along with the continuous growth to derivative demands such as polypropylene, the whole world rapidly increases the demand of propylene.In some areas, such as China, the propylene market value is far above other lower carbon number hydrocarbons.Catalytic cracking also is to produce the especially important technology of propylene of light olefin except producing light Fuel oil productions such as gasoline, diesel oil.At present, the propylene feedstocks in the whole world about 32% originates from catalytic cracking process.Improve though above technology has been carried out some to riser reactor, overcome many deficiencies of conventional riser reactor, do not consider to excavate to greatest extent the potentiality of catalytic cracking propylene-increasing.
More catalytic cracking unit mainly is to contain the catalyzer with MFI structural zeolite by use at present, changes the reaction conditions increase scission reaction degree of depth simultaneously and increases light olefin and productivity of propylene.
A kind of method of producing propylene by catalytic cracking or thermal naphtha material selectivity is disclosed among the CN1383448A.Be boiling point to be contacted less than the zeolite catalyst of about 0.7 nanometer greater than 180 ℃ carbon raw material and the mean pore size that contains 10～50 heavy % form pre-coked catalyst.In described second district, under the reaction conditions of the weight ratio 4～10 of 500～600 ℃ of temperature, hydrocarbon partial pressure 0.07～0.27MPa, 1～10 second residence time and catalyzer and stock oil, petroleum naphtha is contacted with described pre-coked catalyst form crackate, wherein productivity of propylene is up to 16.8 heavy %.
Though above technology is obtaining apparent in view progress aspect the increase catalytic cracking productivity of propylene, but all mainly be to rely on the liquefied gas yield that improves catalytic cracking to improve propene yield, owing to be subjected to the restriction of drastic cracking, isomerization, aromizing and hydrogen transfer reactions under the catalytic cracking reaction condition, its limitation that increases catalytic cracking unit propylene selectivity and productive rate is still very big.
Summary of the invention
The objective of the invention is on the basis of existing technology, providing a kind of is that catalytic material transforms the method for producing propylene with the light hydrocarbons that does not contain propylene.
Method provided by the invention is as follows: riser reactor is co-axial each other first reaction zone, second reaction zone, optional outlet area and level pipe from bottom to up successively, link to each other with settling vessel by level pipe at the outlet area end, first reaction zone is connected two catalyst inlet pipes respectively with the second reaction zone bottom; The unstripped gas of preheating is injected a riser reactor that comprises two reaction zones, enter first reaction zone with the catalyst mix of heat, under 150～450 ℃ temperature of reaction, carry out building-up reactions, and then and the catalyst mix of another part heat enter second reaction zone, under 450～650 ℃ temperature of reaction, carry out cracking and dehydrogenation reaction, after reaction was finished, separated product and reclaimable catalyst, reclaimable catalyst Returning reactor after regenerating recycled.
In the method provided by the invention, described operational condition is: first reaction zone temperature is 150～450 ℃, and preferred 250～450 ℃, reaction times are 0.5～2.0 second, and the weight ratio of preferred 1～2.0 second, catalyzer and unstripped gas is 1～30, preferred 3～21; Second reaction zone temperature is 450～650 ℃, and preferred 480～600 ℃, reaction times are 3～20 seconds, and preferred 3～10 seconds, the weight ratio of catalyzer and unstripped gas was 3～60, preferred 5～40; Absolute pressure is 0.1～0.4MPa in the reactor, preferred 0.15～0.35MPa.
In the method provided by the invention, described catalyzer by first reaction zone bottom introducing reactor is that regenerated catalyst is or/and by the reclaimable catalyst of drawing in other catalyst cracker, the catalyzer of being introduced by the second reaction zone bottom is a regenerated catalyst.
The aspect ratio of first reaction zone of described riser reactor, second reaction zone and outlet area is 10～40:90～60:0～25.
In the method provided by the invention, described riser reactor be the equal diameter riser tube, etc. linear speed riser tube or reducing riser reactor, preferred reducing riser reactor.
Its intermediate diameters riser tube is identical with the catalyst cracker of refinery's routine, waits in the linear speed riser tube fluidic linear speed basic identical; If select the reducing riser reactor for use, the diameter of this reactor first reaction zone, second reaction zone, outlet area is than being 1:1.5～5.0:0.8～1.5.
The diameter of second reaction zone of reducing riser reactor is bigger than the diameter of first reaction zone, and the effect of second reaction zone that the diameter change is big is the flow velocity that reduces carburet hydrogen and catalyzer, under higher temperature of reaction, improves the degree of depth of reactant cracking reaction.
In the method provided by the invention, the temperature of reaction of first reaction zone is lower than the temperature of reaction of conventional catalytic cracking, help light olefin and carry out building-up reactions, by regulating the temperature of unstripped gas, perhaps in the middle of the catalyst inlet pipe, increase cooling tank and regulate the temperature that the catalyst temperature that enters first reaction zone is controlled first reaction zone.The catalyzer of being introduced reactor by first reaction zone bottom can be a regenerator, also can be the reclaimable catalyst of drawing in other catalyst cracker.
In the method provided by the invention, the temperature of the second reaction zone internal reaction thing gas and catalyzer is higher than the temperature of reaction of conventional catalytic cracking or identical with the temperature of reaction of conventional catalytic cracking, helps further cracking of superimposed product and dehydrogenating propane and generates propylene.By controlling the temperature of second reaction zone by the continuous compensation regeneration agent in the second reaction zone bottom, improve catalyzer cracking reaction activity thereby reach, the superimposed product of cracking carries out the purpose of dehydrogenation reaction, and logistics is longer in this reaction zone residence time, is 3～20 seconds.
In the method provided by the invention, the effect of outlet area is to suppress cracking reaction and heat cracking reaction, improves rate of flow of fluid.
In the method provided by the invention, an end of level pipe links to each other with outlet area, and the other end links to each other with settling vessel; When the height of outlet area is 0 to be riser reactor when not having outlet area, and an end of level pipe links to each other with second reaction zone, and the other end links to each other with settling vessel.The effect of level pipe is that product that reaction is generated and reclaimable catalyst are delivered to separation system and carry out gas solid separation.
In the method provided by the invention, reaction product and reclaimable catalyst can adopt conventional gas-solid separation equipment, separate such as conventional cyclonic separator, and the present invention has no particular limits it.
In the method provided by the invention, can adopt conventional gas fractionation plant with the isolating reaction product of reclaimable catalyst, separate such as the conventional gas separation column, isolate propylene, the present invention has no particular limits it.
In the method provided by the invention, revivifier can adopt the fluid bed regenerator of conventional catalytic cracking, cat-cracker, and the present invention has no particular limits it.The effect of revivifier is that spent agent is carried out coke burning regeneration, and the required heat energy of reaction in the reactor is provided.The regeneration of catalyzer is exactly that with the process that the coke in the catalyst mixture is burnt, its operating method and operational condition also are similar to catalytic cracking regenerators such as routine in oxygen-containing atmosphere (being generally air).This process is to well known to a person skilled in the art general knowledge.For example, in general, described regeneration temperature is 600～770 ℃, preferred 650～730 ℃.
In the method provided by the invention, described unstripped gas is the C that isolates behind the propylene
2～C
7The mixture of hydrocarbon comprises the lighter hydrocarbons product that various oil refining or chemical process are produced, and wherein preferred raw material is to have removed propylene, be rich in C
4The hydrocarbon gas of cut comprises C
4And following alkane, alkene and alkynes.
In the method provided by the invention, described unstripped gas is injected separately by reactor lower part, perhaps with lifting medium mixing injecting reactor, promote the mixture that medium comprises water vapor, catalytic cracking or catalytic pyrolysis dry gas, nitrogen one of them or they, the lifting medium of injecting reactor and the weight ratio of unstripped gas are 0～0.15:1.
In the method provided by the invention, described activity of such catalysts component is selected from Y type and modified product thereof and has one or more mixture in the supersiliceous zeolite of five-membered ring structure, or various mixture of catalysts, the preferred catalyzer that contains ZSM-5 zeolite and y-type zeolite simultaneously.
The advantage that light hydrocarbons provided by the invention is produced propylene is:
Adopt method of the present invention, utilize the equipment component of the original riser tube reaction-regeneration system of catalytic cracking, use comprises the riser reactor of two reaction zones, reinforced low-carbon hydrocarbon building-up reactions, the further scission reaction of superimposed product and dehydrogenating propane reaction successively is converted into the propylene with higher economic worth with the less light hydrocarbons of economic worth after gas separation system is isolated propylene under the differential responses condition.
Description of drawings
1-unstripped gas pipeline;
2-first reaction zone;
3-second reaction zone;
The 4-outlet area;
The 5-level pipe;
The 6-second reaction zone lower catalytic agent inlet tube;
The 7-first reaction zone lower catalytic agent inlet tube.
Below in conjunction with accompanying drawing method provided by the present invention is further described.
The mixture of unstripped gas and lifting medium is through the bottom of pipeline 1 injecting lift pipe the first reaction zone 2, the catalyst inlet pipe 7 of catalyst through the first reaction zone bottom of heat enters the first reaction zone, unstripped gas mixes with thermocatalyst and moves upward, after carrying out building-up reactions under 150～450 ℃ the reaction temperature, enter second reaction zone 3, mix with the high-temperature regenerated catalyst of introducing through catalyst inlet pipe 6 again, under 450～650 ℃ reaction temperature, carry out cracking and dehydrogenation reaction, product and green coke decaying catalyst mixture enter piece-rate system through outlet 4 and horizontal tube 5 and carry out gas solid separation, reclaimable catalyst enters regenerator and carries out coke burning regeneration, and product is then separated through the oil-gas pipeline body piece-rate system of degassing.
Embodiment
The following examples will give further instruction to the present invention, but be not therefore and restriction the present invention.
The structure of the riser reactor of employed medium-scale is as follows in embodiment, the Comparative Examples:
The total height of equal diameter riser reactor is 12 meters, and diameter is 0.25 meter, and wherein the first reaction zone height is 4.4 meters, and the second reaction zone height is 5.2 meters; The outlet area height is 2.4 meters.
The total height of reducing riser reactor is 12 meters, and first reaction zone diameter is 0.25 meter, and it highly is 4.4 meters; Second reaction zone diameter is 1 meter, and it highly is 5.2 meters; The diameter of outlet area is 0.25 meter, and it highly is 2.4 meters.
Employed catalyzer is produced by China Petrochemical Corp.'s Shandong catalyst plant, and character is listed in the table 1.
Employed raw material is a C 4 fraction, and its character is listed in table 2.
Comparative Examples
This Comparative Examples is on equal diameter riser tube reaction-regeneration system, with C
4Cut is a raw material, uses catalyzer CRP-1 to carry out the method for conventional catalyzed conversion.
Main operational condition and product distribute and list in table 3.
By table 3 data as seen, productivity of propylene is 9.16 heavy %.
Present embodiment is on equal diameter riser tube reaction-regeneration system, with C
4Cut is a raw material, uses catalyzer CRP-1 to carry out the method for catalyzed conversion.
The unstripped gas of preheating is injected a riser reactor that comprises two reaction zones, be mixed into first reaction zone with the catalyzer CRP-1 of heat, under 280 ℃ average reaction temperature, carry out building-up reactions, and then and the catalyzer CRP-1 of another part heat be mixed into second reaction zone, under 590 ℃ average reaction temperature, carry out cracking and dehydrogenation reaction, after reaction was finished, separated product and reclaimable catalyst, reclaimable catalyst Returning reactor after regenerating recycled.Main operational condition and product distribute and list in table 3.
By table 3 data as seen, productivity of propylene is 23.77 heavy %.
Present embodiment is on equal diameter riser tube reaction-regeneration system, with C
4Cut is a raw material, uses catalyzer MLC-500 to carry out the method for catalyzed conversion.
The unstripped gas of preheating is injected a riser reactor that comprises two reaction zones, be mixed into first reaction zone with the catalyzer MLC-500 of heat, under 300 ℃ average reaction temperature, carry out building-up reactions, and then and the catalyzer MLC-500 of another part heat be mixed into second reaction zone, under 590 ℃ average reaction temperature, carry out cracking and dehydrogenation reaction, after reaction was finished, separated product and reclaimable catalyst, reclaimable catalyst Returning reactor after regenerating recycled.Main operational condition and product distribute and list in table 3.
By table 3 data as seen, productivity of propylene is 15.25 heavy %.
Present embodiment is on reducing riser tube reaction-regeneration system, uses catalyzer CRP-1 to carry out the method for catalyzed conversion.
The unstripped gas of preheating is injected a riser reactor that comprises two reaction zones, be mixed into first reaction zone with the catalyzer CRP-1 of heat, under 350 ℃ average reaction temperature, carry out building-up reactions, and then and the catalyzer CRP-1 of another part heat be mixed into second reaction zone, under 500 ℃ average reaction temperature, carry out cracking and dehydrogenation reaction, after reaction was finished, separated product and reclaimable catalyst, reclaimable catalyst Returning reactor after regenerating recycled.Main operational condition and product distribute and list in table 3.
By table 3 data as seen, productivity of propylene is 28.24 heavy %.
Present embodiment is on reducing riser tube reaction-regeneration system, uses catalyzer CRP-1 to carry out the method for hydrocarbon ils catalyzed conversion.
The unstripped gas of preheating is injected a riser reactor that comprises two reaction zones, be mixed into first reaction zone with the catalyzer CRP-1 of heat, under 300 ℃ average reaction temperature, carry out building-up reactions, and then and the catalyzer CRP-1 of another part heat be mixed into second reaction zone, under 590 ℃ average reaction temperature, carry out cracking and dehydrogenation reaction, after reaction was finished, separated product and reclaimable catalyst, reclaimable catalyst Returning reactor after regenerating recycled.Main operational condition and product distribute and list in table 3.
By table 3 data as seen, productivity of propylene is 33.65 heavy %.
Table 1
| The catalyzer trade names | CRP-1 | MLC-500 |
| Active ingredient | ZRP+USY | REUSY |
| Chemical constitution, heavy % | ||
| Al 2O 3 | 54.2 | 54.1 |
| Na 2O | 0.03 | 0.20 |
| Specific surface, m 2/g | 160 | 252 |
| Pore volume (water droplet method), ml/g | 0.26 | 0.35 |
| Tap density, ml/g | 0.86 | 0.69 |
| Abrasion index, m%/h | 1.2 | 1.5 |
| *Micro-activity after the burin-in process | 64 | 65 |
*The hydrothermal aging condition of catalyzer is 800 ℃, 100% water vapor, 12 hours.
Table 2
| Raw material is formed | Content, heavy % |
| Propane | 13.11 |
| Propylene | 1.40 |
| Trimethylmethane | 14.35 |
| Normal butane | 7.64 |
| Butene-1 | 11.91 |
| Iso-butylene | 26.87 |
| Instead-butylene | 14.82 |
| Suitable-butylene | 9.90 |
| Amount to | 100.00 |
Table 3
Claims (13)
1, a kind of catalysis conversion method of producing more propylene, it is characterized in that riser reactor is co-axial each other first reaction zone, second reaction zone, optional outlet area and level pipe from bottom to up successively, level pipe links to each other with settling vessel, and first reaction zone is connected the catalyst inlet pipe respectively with the second reaction zone bottom; The unstripped gas of preheating is injected a riser reactor that comprises two reaction zones, enter first reaction zone with the catalyst mix of heat, under 150～450 ℃ temperature of reaction, carry out building-up reactions, and then and the catalyst mix of another part heat enter second reaction zone, under 450～650 ℃ temperature of reaction, carry out cracking and dehydrogenation reaction, after reaction was finished, separated product and reclaimable catalyst, reclaimable catalyst Returning reactor after regenerating recycled.
2, according to the method for claim 1, the reaction times that it is characterized in that described first reaction zone is 0.5～2.0 second, and the weight ratio of catalyzer and unstripped gas is 1～30; The reaction times of second reaction zone is 3～20 seconds, and the weight ratio of catalyzer and unstripped gas is 3～60; Absolute pressure is 0.1～0.4MPa in the reactor.
3, according to the method for claim 1, it is characterized in that by the catalyzer that reactor is introduced in the first reaction zone bottom be regenerated catalyst or/and the reclaimable catalyst of drawing in other catalyst cracker, the catalyzer of being introduced by the second reaction zone bottom is a regenerated catalyst.
4,, it is characterized in that the aspect ratio of first reaction zone, second reaction zone and the outlet area of described riser reactor is 10～40:90～60:0～25 according to the method for claim 1.
5, according to the method for claim 1, it is characterized in that described riser reactor be the equal diameter riser tube, etc. linear speed riser tube or reducing riser reactor.
6, according to the method for claim 5, the diameter of first reaction zone, second reaction zone, outlet area that it is characterized in that described reducing riser reactor is than being 1:1.5～5.0:0.8～1.5.
7, according to the method for claim 2, it is characterized in that described reaction conditions is 250～400 ℃ of first reaction zone temperatures, 1～2.0 second reaction times, the weight ratio of catalyzer and unstripped gas is 3～21; 480～600 ℃ of the temperature of second reaction zone, 3～10 seconds reaction times, the weight ratio of catalyzer and unstripped gas is 5～40; Absolute pressure is 0.15～0.35MPa in the reactor.
8,, it is characterized in that described activity of such catalysts component is selected from one or more the mixture in Y type or HY type zeolite, the ultrastable Y that contains or do not contain rare earth, ZSM-5 zeolite that contains or do not contain rare earth or the supersiliceous zeolite with five-membered ring structure according to the method for claim 1.
9,, it is characterized in that described catalyzer contains ZSM-5 zeolite and y-type zeolite simultaneously according to the method for claim 8.
10,, it is characterized in that described unstripped gas is the C that isolates behind the propylene according to the method for claim 1
2～C
7The mixture of hydrocarbon.
11,, it is characterized in that described unstripped gas is to be rich in C according to the method for claim 10
4The hydrocarbon gas of cut.
12, according to the method for claim 1, it is characterized in that described unstripped gas injects separately from reactor lower part, perhaps, promote medium and be selected from wherein one or more mixture of water vapor, catalytic cracking or catalytic pyrolysis dry gas, nitrogen with lifting medium mixing injecting reactor.
13,, it is characterized in that the lifting medium of injecting reactor and the weight ratio of unstripped gas are 0～0.15 according to the method for claim 12.
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| CNB2005100898504A CN100537713C (en) | 2005-08-09 | 2005-08-09 | A kind of catalysis conversion method of producing more propylene |
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| CN100537713C true CN100537713C (en) | 2009-09-09 |
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| US8246914B2 (en) | 2008-12-22 | 2012-08-21 | Uop Llc | Fluid catalytic cracking system |
| CN102531824B (en) * | 2011-12-29 | 2014-07-16 | 北京惠尔三吉绿色化学科技有限公司 | Process method for preparing propylene and ethylene from liquid gas including butylene |
| CN108620017A (en) * | 2018-06-06 | 2018-10-09 | 江苏联合创业环保有限公司 | Thermal cracking integration apparatus |
| CN114173919B (en) * | 2019-07-30 | 2024-01-16 | 国际壳牌研究有限公司 | riser reactor system |
| CN112552957B (en) * | 2019-09-25 | 2022-03-11 | 中国石油化工股份有限公司 | Method for recycling and cracking hydrocarbons |
| CN115364775B (en) * | 2022-08-17 | 2024-04-12 | 山东高端化工研究院有限公司 | Device for controlling reaction temperature in olefin preparation by crude oil catalytic pyrolysis |
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