CN1217366A - Catalyst cracking method for producing in high-yield olefin and lift-leg reaction system thereof - Google Patents
Catalyst cracking method for producing in high-yield olefin and lift-leg reaction system thereof Download PDFInfo
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- CN1217366A CN1217366A CN 97120272 CN97120272A CN1217366A CN 1217366 A CN1217366 A CN 1217366A CN 97120272 CN97120272 CN 97120272 CN 97120272 A CN97120272 A CN 97120272A CN 1217366 A CN1217366 A CN 1217366A
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Abstract
The fluidized-bed catalytic cracking process for prolifically producing low-carbon isomeric olefin or propylene is implemented in the lift pipe reaction system comprising the following two portions: 1. a lift pipe reactor improved and formed by prelifting stage and three-stage reaction zones divided along the height of bed layer; and 2. a gas-solid quick separation system formed from downgoing bed containing multi-stage cover-type porous gas-solid separation structure and closed cyclone separator. As compared with conventional FCC method, said invention can obtain higher low-carbon isomeric olefin and propylene yield.
Description
The invention relates to producing in high-yield olefin, the fluidized catalytic cracking method of particularly voluminous low-carbon (LC) isomeric olefine or propylene and used riser tube reactive system thereof.
Along with social demand to the raising of product requirement and the heaviness of raw material, people are also improving constantly the requirement of catalytic cracking technology.In order to satisfy the needs of reformulated gasoline to ethers oxygenatedization thing, require to increase the output of low-carbon (LC) isomeric olefine, oil refining and chemical industry combination closely day by day make many refinery requirement propylene enhancings; The heaviness of raw material forces the reaction unit of refinery to mix refining atmospheric residue and vacuum residuum at large, and for this reason, new catalytic cracking process and catalyzer constantly are developed, and reaction unit correspondingly also constantly is updated and is perfect.
In catalytic cracking 50 years of development, no matter riser reactor has still all obtained significant progress from structure on operating method.This shows that mainly mixing, outlet product rapid of feed zone oil gas and catalyzer separates, reduces on the riser tube cross section thermograde and reduce aspect such as back-mixing.Specifically the major progress of relevant this respect is as follows:
Aspect the mixing of feed zone, improve on the oil gas catalyzer contact efficiency that mainly concentrates on the constantly perfect of nozzle and raising charging position initial segment.The improvement of nozzle mainly develops towards directions such as low pressure drop, homodisperse, little droplet dia and homogeneous droplet diameter distribution, can be referring to relevant patent USP4 for example, and 434,049, USP4,427,537, CN8801168, EP546,739 etc.
USP4 has described a kind of method of improving oil gas and catalyst mix in 717,467, that is: regenerated catalyst enters mixing section by inclined tube, and mixing section is coaxial and straight tube different diameter is formed by two, and the caliber of bottom is less than the caliber on top.The pre-gas that promotes is entered by the bottom straight tube, carries catalyzer and enters the top straight tube, thereby catalyzer is entered by the riser tube center.Oil gas is by injecting along promoting the tube edge wall around the outlet of top straight tube.Catalyzer and oil gas so the mode of entrance radial distribution of having improved charging position initial segment inner catalyst contact with oil gas, but be not improved aspect uniformity coefficient that strengthens oil gas and catalyst mix and the mixture strength.
USP5,318, proposed to improve the method for charging position initial segment oil gas and catalyst mix efficient in 691, being regenerated catalyst enters a deceleration area by pre-lifting from the interannular of initial segment, by the generation vortex motion of uprushing of pipeline section, oil gas promptly radially sprays into riser tube in the central zone of this section in this deceleration area.Strengthen the mixture strength of oil gas and catalyzer initial segment thus by vortex motion, strengthen the condensation rate of oil gas and reduce green coke.But from another angle, because the generation of vortex motion has increased the back-mixing of catalyzer, thereby can not guarantee that fresh feed contacts with the high temperature regeneration agent, this is extremely disadvantageous to reaction.
USP4 has proposed a kind of feed process that improves oil gas and catalyzer in 650,566.This method is to inject oil gas by a plurality of nozzles that are evenly distributed on the feed zone cross section, each nozzle all comes dominant discharge by independent pipeline and valve, temperature distribution by monitoring riser tube cross section, regulate the relative discharge of oil gas on each pipeline, the reaction on each cross section is in same intensity in the riser tube thereby make.
USP4 has proposed to improve by the mode of sectional feeding the method for product gasoline octane value in 869,807 in traditional riser reactor.For example first opening for feed enters from the bottom with the stock oil more than 50%, and rest part enters from second opening for feed.
USP5 has proposed the method for multistage reaction in 154,818, and be about to riser reactor and be divided into two conversion zones: reclaimable catalyst and lightweight material are advanced in the first area, and second area at an upper portion thereof advances live catalyst and heavy feed stock.This method all has positive effect to reducing a pair product yield, raising purpose product production and gasoline octane rating aspect.
USP5 has proposed a kind of new feed process in 139,748, and promptly oil gas is sprayed on mobile granules of catalyst along the direction that is substantially perpendicular to the riser tube axis, thereby shortens the mixinglength of initial segment, has improved quality product.
Cracking is crossed in inhibition riser tube exit and heat cracking reaction is the focus that people research and develop.Now mainly contain two technological lines, one is the gas-solid sharp separation that adopts outlet, and another is the method that adopts the outlet cold shock.
People study the more two kinds of forms that have in the technological line of gas-solid sharp separation: the enclosed cyclonic separation is separated with uncovered ejection type.EP162,978 have proposed the enclosed cyclone separation method of riser tube outlet, are about to two elementary cyclonic separators and directly are bound up on the sharp separation that gas-solid is realized in the riser tube exit, thereby reach the raising separation efficiency, reduce product and cross the cracked purpose.
EP139, a kind of method of pressure wave with stable operation that produce that overcome in the enclosed cyclone separation system then proposed in 392, promptly the different sites in cyclone separation system is installed flutter valve, thereby the variation of the pressure different opening degrees that can directly change flutter valve avoid producing pressure wave like this.Adopting the advantage of enclosed cyclone separation method is to have than high separating efficiency, reduced the cracking of crossing of product, but the problem that exists is easily coking in connecting portion and the cyclonic separator, and owing in fact separate chamber's volume does not reduce, thereby heat scission reaction is not controlled.
EP564 has proposed a kind of uncovered ejection type partition method in 678 and USP5,104,517.This method is to utilize gas-solid to be used to the difference of power, and the promotion by pressure reduction separates gas-solid rapidly.Thereby this method has reduced the volume of segregation section effectively and has reduced thermally splitting, can also improve stripping stage dense bed height simultaneously.
USP5 has proposed the separation method of the uncovered ejection type of a kind of plug flow in 308,474.In the method, the opening of collector is positioned at the collector bottom around the riser tube, thereby makes oil gas and catalyzer keep the same flow direction after outlet.Like this, segregation section has played effectively under the prerequisite that does not influence separation efficiency and has been used to control the gas-solid purpose of duration of contact.
Another suppresses riser tube outlet back crosses the cracked technological line and promptly exports cold shock, such as USP5, all this method is described in the patent such as 089,235.Because the method for outlet cold shock can reduce the temperature out of reactant flow rapidly, therefore can suppress cracking effectively.But being the load that causes follow-up pneumatic press, its subject matter increases, and because cold shock has also reduced the temperature of catalyzer simultaneously, so caused unnecessary thermosteresis.
EP593 has proposed a kind of gas solid separation that realizes effectively in 823, only makes the method for split product cold shock simultaneously.In the method, the streams of coming out from riser tube reaches the rapid separation of gas-solid by a centrifugal separator tube.Catalyzer falls along wall; The cold shock medium then is sprayed on the oil gas phase by a nozzle, and the selection by nozzle can make the cold shock medium form certain thickness fan-shaped plan.
Though riser reactor has been obtained the progress of above-mentioned each side, also have many local improvement and perfect that need.Particularly, must reform existing riser tube reactive system in order to realize the catalytic cracking process target of low-carbon olefines high-output.Because with regard to the characteristics of this technology, because the raw materials used heavy distillate of mixing residual oil that mostly is, its carbon residue and boiling point are higher, thereby easily cause catalyzer coking inactivation.Consider that from the viewpoint of reaction kinetics in order to reach the purpose of low-carbon olefines high-output, reaction needs higher response intensity, promptly higher temperature of reaction and agent-oil ratio in earlier stage; And need suitably to reduce response intensity to suppress hydrogen transference and to cross cracking etc. and pay reaction in the reaction later stage.In addition, in order to prevent the generation of crossing cracking and heat scission reaction after riser tube outlet, the termination reaction and realize the rapid separation of gas-solid as early as possible at riser tube outlet position.
Said process will produce following problem as carrying out on traditional riser tube reaction unit:
1. the catalyst in reactor radial distribution is inhomogeneous, the trend that the oriented wall of particle compiles.Cause the granules of catalyst concentration distribution of center dilute phase, the close phase of near wall region thus, and then cause in riser tube agent-oil ratios different on the same cross section.Consequently the near wall region response intensity is stronger, the central section response intensity a little less than, cannot or hardly really control the reaction conditions in the riser tube in the operation.
Since granules of catalyst in reactor inside diameter to the ununiformity that distributes, cause being in the reactor internal recycle mobile gas, fixed double phase flow structure, promptly be that particle upwards flows in the bed centre, and be that particle flows downward near wall region, it is unfavorable greatly that this phenomenon of solid back-mixing largely is to purpose that the catalytic cracking process of low-carbon olefines high-output brings, that is: at the pre lift zone of riser tube, the low temperature catalyst that landing is got off contacts with stock oil and causes the latter not vaporize, and then produces coke.Simultaneously because the landing of catalyzer causes the temperature inequality of catalyzer on the same cross section, and then cause response intensity than big-difference.
At riser tube outlet position because the solid back-mixing and the long residence time, cross cracking, thermally splitting and hydrogen transference etc. and pay reaction and will reduce the productive rate of purpose product greatly.Generally at the settling vessel dilute phase space, isomeric olefine has 40～50% approximately by the saturated isoparaffin that is converted into of hydrogen transference.
Purpose of the present invention promptly is in order to overcome the deficiencies in the prior art, a kind of producing in high-yield olefin, the particularly fluidized catalytic cracking method of low-carbon (LC) isomeric olefine or propylene to be provided on the basis of above-mentioned prior art.
Another object of the present invention then provide a kind of fluidized catalytic cracking method that is applicable to this producing in high-yield olefin improvement the riser tube reactive system.
Fluidized catalytic cracking method provided by the invention comprises that the purpose product is that low-carbon (LC) isomeric olefine and purpose product are the embodiment of propylene.Certainly, if fluid catalytic cracking embodiment provided by the invention is applied in traditional fluid catalytic cracking process, then will obtain significant effect aspect yield that improve product gasoline and the quality.
One, the fluidized catalytic cracking method of voluminous isomeric olefine
For the purpose product is the fluid catalytic cracking of low-carbon (LC) isomeric olefine, and method provided by the invention is such:
As shown in Figure 1, one by pre lift zone [1] and three sections reaction zones [2,3,4] in the riser reactor of Gou Chenging, the partial regeneration agent is respectively via the bottom with after twice lifting of the gaseous media that tangentially enters, with mix by a charging oil gas that radially sprays into and enter radial shrinkage immediately first reaction zone, after 0.5～1.0 second the residence time, enter radially the second reaction zone bottom of having expanded than first reaction zone.At this position, the lifting of the gaseous media of another part regenerator through tangentially entering along axle, with mix by the secondary feeds oil gas that radially sprays into and from the logistics of first reaction zone after enter radial shrinkage immediately second reaction zone, after 0.5～1.0 second the residence time, enter the 3rd reaction zone that is positioned at the riser tube horizontal section, and the cold shock medium is injected wherein.Logistics is 0.5～1.0 second in the 3rd reaction zone to the residence time that exports the position, and the total residence time in the riser tube reactive system is 1.0～2.0 seconds.Educt flow after the cold shock enters one to have the separation system that the descending bed of continuous multi-stage gas solid separation structure forms by enclosed cyclonic separator and and carries out gas solid separation, isolated gas phase is drawn by the outlet of cyclonic separator, and granules of catalyst enters revivifier through stripping.
According to aforesaid method provided by the invention, the purpose of voluminous low-carbon (LC) isomeric olefine is to reach in a novel riser tube reactive system of being made up of riser reactor that has improved and custom-designed separation system.
This riser reactor that has improved is to be made of pre lift zone [1] and three sections reaction zones [2,3,4].
In pre lift zone [1], account for regenerator circulation total amount below 50% from revivifier, be preferably 10～40%, be preferably 15～35% regenerator and enter, and entered by gas inlet [6] and pre-lifting of gaseous media institute by bottom sparger [7] by inclined tube [5].For the stock oil drop and the high temperature regeneration agent of coming out from nozzle are mixed, improve mixing efficiency, reach the instant vaporization of drop, also contact the purpose of strengthening initial cracking reaction to reach with carbon-bearing catalyzer that fall after rise, that surface temperature is lower simultaneously in order to reduce stock oil as far as possible, except that the pre-lifting of above-mentioned routine, promote once more along the tangential gaseous media that feeds no more than lift gas total amount 1/3 of axle by gas jet [8] in a feed nozzle [9] below.Used gaseous media is generally water vapor or dry gas that catalytic cracking unit produced, gas speed general requirement makes the flow state in the riser tube maintain turbulent flow between the state of fast fluidized bed, and making the volumetric concentration of granules of catalyst in pre lift zone is that solid holdup is controlled at 0.15～0.4, preferably between 0.2～0.3.
After catalyzer is promoted to certain altitude, the relative mixture of desiring to mix as reaction raw materials than light constituent (vacuum gas oil) with small part of whole heavy component (VACUUM TOWER BOTTOM oil) radially sprays into pre lift zone and catalyst mix by a feed nozzle [9], and enter radial shrinkage immediately in the lump first reaction zone and in this district, stop and carried out a cracking reaction in 0.5～1.0 second.Inlet amount by a feed nozzle generally accounts for below 60% of total feed, is preferably 10～50%, is preferably 20～40%.This reaction zone is high zone of transformation of cracking of high severity, and its effect mainly is the abundant cracking that guarantees heavy feed stock.
Be advanced into radially the second reaction zone bottom of having expanded than first reaction zone [10] on continuing from the streams of first reaction zone.Account for regenerator circulation total amount more than 50% at this position from revivifier, be preferably 60～90%, be preferably 65～85% regenerator and enter by inclined tube [11], and by by be positioned at secondary feeds nozzle [13] below by gas jet [12] along the tangential gaseous media institute homodisperse that feeds of axle and promote.Gaseous media still is water vapor or dry gas.The purpose that enters most of regenerator once more by inclined tube [11] is that blending ratio by regulating part catalysts and regenerator is with the activity of conditioned reaction device inner catalyst.
Most ofly in the reaction raw materials radially spray into the second reaction zone bottom by secondary feeds nozzle [13], and mix from the streams of first reaction zone and from inclined tube [11] and the regenerator that disperseed, promoted than light constituent (vacuum gas oil).Mixed streams enter radial shrinkage immediately second reaction zone [3] and in this district, stop and carried out the secondary cracking reaction in 0.5～1.0 second.Inlet amount by the secondary feeds nozzle generally accounts for more than 40% of total feed, is preferably 50～90%, is preferably 60～85%.The effect of suitable reduction temperature of reaction has not only been played in the injection of secondary feeds, and be the agent-oil ratio of regulating second reaction zone, the important means that improves reaction preference, owing to certainly will cause violent secondary cracking after entering second reaction zone from the crackate of first reaction zone, comprising a large amount of hydrogen transferences and cross cracking etc. and pay reaction, therefore must suppress the secondary cracking reaction by the injection of fresh low temperature feedstock.
The streams of being come out by second reaction zone enters the 3rd reaction zone [4] that is positioned at the riser tube horizontal section along riser reactor.In this reaction zone, the liquid medium that is used for cold shock and termination cracking reaction is injected by inlet [14].Pay reaction to reduce response intensity, increase isomerization reaction, minimizing hydrogen transference etc.As the liquid medium of cold shock must possess cooling fast, make the fast performance of poisoning of catalyst inactivation, and should try one's best and not increase the load of pneumatic press.For this reason, the liquid medium that adopts among the present invention is selected from coker gas oil, coking gasoline and diesel or dilution and the slurry oil through fully having atomized.In this reaction zone, the structure of streams is that up, level and descending conveying series connection constitute.
Streams tangentially enters the descending bed [15] in the separation system after through the 3rd reaction zone, rely on action of centrifugal force, granules of catalyst falls into stripping stage [16] by descending bed outlet, oil gas then in descending bed multistage bell-type porous gas solid separation structure [17] tell by enclosed cyclonic separator [18].Streams in the 3rd reaction zone to the residence time that arrives descending bed outlet be 0.5～1.0 second, total residence time in the riser tube reactive system was advisable with 1.0～20 seconds, can be when implementing the particular case of raw material and catalyzer, be optimized definite by reaction kinetics.
In the riser tube reactive system that has improved provided by the invention, the hybrid density of oil gas and regenerator respectively is ρ 1, ρ 2, ρ 3 and ρ 4 in these four positions of pre lift zone, first reaction zone, second reaction zone and the 3rd reaction zone.Be in the fluid catalytic cracking of purpose product with the low-carbon (LC) isomeric olefine, this density distribution is advisable with ρ 1＞ρ 3＞ρ 2 ≈ ρ 4.
Two, the fluidized catalytic cracking method of producing more propylene
For the purpose product is the fluid catalytic cracking of propylene, and method provided by the invention is such:
As shown in Figure 1, one by pre lift zone [1] and three sections reaction zones [2,3,4] in the riser reactor of Gou Chenging, the partial regeneration agent is respectively via the bottom with after twice lifting of the gaseous media that tangentially enters, with mix by a charging oil gas that radially sprays into and enter radial shrinkage immediately first reaction zone, after 05～1.0 second the residence time, enter radially the second reaction zone bottom of having expanded than first reaction zone.At this position, the lifting of the gaseous media of another part regenerator through tangentially entering along axle, with mix by the secondary feeds oil gas that radially sprays into and from the logistics of first reaction zone after enter radial shrinkage immediately second reaction zone, after 1.0～1.5 seconds the residence time, enter the 3rd reaction zone that is positioned at the riser tube horizontal section, and the cold shock medium is injected wherein.Logistics is 0.5～1.0 second in the 3rd reaction zone to the residence time that exports the position, and the total residence time in the riser tube reactive system is 2.0～4.5 seconds.Educt flow after the cold shock enters one to have the separation system that the descending bed of continuous multi-stage gas solid separation structure forms by enclosed cyclonic separator and and carries out gas solid separation, isolated gas phase is drawn by the outlet of cyclonic separator, and granules of catalyst enters revivifier through stripping.
According to aforesaid method provided by the invention, the purpose of producing more propylene is to reach in a novel riser tube reactive system of being made up of riser reactor that has improved and custom-designed separation system as hereinbefore.
In pre lift zone [1], account for regenerator circulation total amount more than 50% from revivifier, be preferably 60～90%, be preferably 65～85% regenerator and enter, and entered by gas inlet [6] and pre-lifting of gaseous media institute by bottom sparger [7] by inclined tube [5].For the stock oil drop and the high temperature regeneration agent of coming out from nozzle are mixed, improve mixing efficiency, reach the instant vaporization of drop, also contact the purpose of strengthening initial cracking reaction to reach with carbon-bearing catalyzer that fall after rise, that surface temperature is lower simultaneously in order to reduce stock oil as far as possible, except that the pre-lifting of above-mentioned routine, promote once more along the tangential gaseous media that feeds no more than lift gas total amount 1/3 of axle by gas jet [8] in a feed nozzle [9] below.Used gaseous media is generally water vapor or dry gas that catalytic cracking unit produced, gas speed general requirement makes the flow state in the riser tube maintain turbulent flow between the state of fast fluidized bed, and making the volumetric concentration of granules of catalyst in pre lift zone is that solid holdup is controlled at 0.15～0.4, preferably between 0.2～0.3.
After catalyzer is promoted to certain altitude, the heavy component of desiring to mix as reaction raw materials (VACUUM TOWER BOTTOM oil) radially sprays into pre lift zone and catalyst mix with relative mixture than light constituent (vacuum gas oil) by a feed nozzle [9], and enter radial shrinkage immediately in the lump first reaction zone and in this district, stop and carried out a cracking reaction in 0.5～1.0 second.Inlet amount by a feed nozzle generally accounts for more than 40% of total feed, is preferably 50～95%, is preferably 60～85%.This reaction zone is high zone of transformation of cracking of severity, and its effect mainly is the abundant cracking that guarantees most of raw material.
Be advanced into radially the second reaction zone bottom of having expanded than first reaction zone [10] on continuing from the streams of first reaction zone.Account for regenerator circulation total amount below 50% at this position from revivifier, be preferably 10～40%, be preferably 15～35% regenerator and enter by inclined tube [11], and by by be positioned at secondary feeds nozzle [13] below by gas jet [12] along the tangential gaseous media institute homodisperse that feeds of axle and promote.Gaseous media still is water vapor or dry gas.The purpose that is entered the high temperature regeneration agent by inclined tube [11] is to increase by the response intensity that improves this moment the cracking of crossing of intermediate product and gasoline product, and makes the further cracking of isopentene.
Another part heavy component and radially spray into the second reaction zone bottom by secondary feeds nozzle [13] than the light constituent mixing raw material and mixes from the streams of first reaction zone and from inclined tube [11] and the regenerator that disperseed, promoted.Mixed streams enter radial shrinkage immediately second reaction zone [3] and in this district, stop and carried out the secondary cracking reaction in 1.0～1.5 seconds.Inlet amount by the secondary feeds nozzle generally accounts for below 60% of total feed, is preferably 10～50%, is preferably 20～40%.
The streams of being come out by second reaction zone enters the 3rd reaction zone [4] that is positioned at the riser tube horizontal section along riser reactor.In this reaction zone, the liquid medium that is used for cold shock and stops cracking reaction is paid reaction by inlet [14] injection to reduce response intensity, minimizing hydrogen transference etc.As the liquid medium of cold shock must possess cooling fast, make the fast performance of poisoning of catalyst inactivation, and should try one's best and not increase the load of pneumatic press.For this reason, the liquid medium that adopts among the present invention is selected from coker gas oil, coking gasoline and diesel or dilution and the slurry oil through fully having atomized.In this reaction zone, the structure of streams is that up, level and descending conveying series connection constitute.
Streams tangentially enters the descending bed [15] in the separation system after through the 3rd reaction zone, rely on action of centrifugal force, granules of catalyst falls into stripping stage [16] by descending bed outlet, oil gas then in descending bed multistage bell-type porous gas solid separation structure [17] tell by enclosed cyclonic separator [18].Streams in the 3rd reaction zone to the residence time that arrives descending bed outlet be 0.5～1.0 second, the total residence time in the riser tube reactive system was advisable with 2.0～4.5 seconds, can be when implementing the particular case of raw material and catalyzer.Be optimized definite by reaction kinetics.
In the riser tube reactive system that has improved provided by the invention, the hybrid density of oil gas and regenerator respectively is ρ 1, ρ 2, ρ 3 and ρ 4 in these four positions of pre lift zone, first reaction zone, second reaction zone and the 3rd reaction zone.Be in the fluid catalytic cracking of purpose product with the propylene, this density distribution is advisable with ρ 1＞ρ 3＞ρ 2＞ρ 4.Three, the riser tube reactive system that has improved
The improvement of the fluidized catalytic cracking method that is applicable to above-mentioned voluminous low-carbon (LC) isomeric olefine or propylene provided by the invention the riser tube reactive system form i.e.: the riser reactor that constitutes by pre lift zone and first, second and third reaction zone of dividing along bed height by two portions; The gas-solid Quick Separation System that constitutes by the descending bed and the enclosed cyclonic separator of the bell-type porous gas solid separation structure that contains multistage.Its structure is as follows:
Be provided with regenerator inlet inclined tube [5], the gas distributor [7] that communicates with gaseous media inlet [6], along being the excessive part [19] of a radial shrinkage between the pre lift zone [1] of a tangential gaseous media nozzle [8] of axle and a feed nozzle [9] and first reaction zone [2] that is positioned at above it, first reaction zone and be positioned at its top second reaction zone [3] between for radial dilatation, be provided with regenerator inlet inclined tube [11], along a tangential gaseous media nozzle [12] and the second reaction zone bottom [10] of secondary feeds nozzle [13], second reaction zone top is to be positioned at the riser tube horizontal section, the end points place is provided with the 3rd reaction zone [4] of liquid medium inlet [14], its outlet is connecting descending bed [15], the inlet tube [20] of enclosed cyclonic separator [18] extends in this descending bed, is the placed in-line bell-type porous of the multistage gas solid separation structure [17] that fuses with it under this extension.
Specifically, as shown in Figure 1, at the gas distributor [7] of the bottom of pre lift zone [1] for communicating with gaseous media inlet [6], inclined tube [5] is the regenerator inlet.Be provided with on the top of pre lift zone along tangential equally distributed 2～8 of perisporium axle, best 3～6 gaseous media nozzles [8], nozzle opening up, axial angle is generally between 20～40 °.The top of gas jet is a feed nozzle [9], and the position of this nozzle generally is controlled at the transition point place between bed emulsion zone and freeboard of fluidized bed.
Pre lift zone and radial shrinkage first reaction zone [2] between be the excessive part [19] of radial shrinkage, feed nozzle promptly is positioned at the below of this constriction, the angle of throat of this constriction generally between 45～80 °, can carry out simulative optimization to it by flow equation and determine by contracted length and angle.
It between identical first reaction zone [2] of radial dimension and second reaction zone [3] the second reaction zone bottom [10] that a diameter has been expanded, be provided with at the position of this expansion regenerator inlet inclined tube [11], with pre lift zone inner nozzle [8] distributes, quantity is all identical gaseous media nozzle [12] and secondary feeds nozzle [13], expansion and hypersystole angle partly requires same pre lift zone.
To help to improve the speed uplink of granules of catalyst and oily vapour gas phase in custom-designed radial shrinkage part between the pre lift zone and first reaction zone and between the second reaction zone bottom and second reaction zone, reduce effectively catalyzer radially concentration gradient contact with the fresh reactant raw material with preventing the downward landing of top catalyzer.Because this contraction, velocity flow profile gets more even; Because shrink the booster action that produces, from the energy conservation viewpoint as can be known, the pressure after the contraction will reduce significantly than perisystolic pressure, this has all prevented the landing and the back-mixing of catalyzer effectively.
Being the 3rd reaction zone [4] that is positioned at the riser tube horizontal section on second reaction zone, is a liquid medium inlet [14] in the end points place of this horizontal section, and the outlet of horizontal section is connecting descending bed [15].The inlet tube [20] of enclosed cyclonic separator [18] extends in the descending bed, is the placed in-line bell-type porous of the multistage gas solid separation structure [17] (hereinafter to be referred as hood configuration) that fuses with it under this extension.
Said hood configuration by pipe core be connected that thereon cover forms.This pipe core is coaxial with the footpath with cyclone inlet pipe [20].This hood configuration can be in series by 4～10 sections, decides on the scale size of descending bed.The initial section of hood configuration should be lower than the position of riser tube horizontal section, and the distance between terminate section and the descending bed bottom end face should be 1～2 times of cyclone inlet pipe diameter.Hood configuration is shown in figure two.Figure middle conductor a promptly represents the hood configuration of single hop, has equally distributed 3～9 apertures of 1～3 row at the cover lower edge of every section hood configuration pipe core perisporium.The total area of all apertures is long-pending 0.3～1.2 times of cyclone inlet tube section on the multistage hood configuration.Angle α between cover and pipe core is 15～45 °.The height H of cover is 3～10 times of hole diameter.The height h of no angle vertical section is about 1/2nd of cover height H on the cover.
So the special device that carries out continuous gas solid separation of design can make lighter hydrocarbons successively by the aperture under the cover, the pipe core of hood configuration, the inlet tube of cyclonic separator, draws in the autoreaction district as soon as possible, realizes gas solid separation rapidly.
Processing method provided by the invention and matching used improved riser tube reactive system thereof have following characteristics:
1. the mode that adopts the part lift gas tangentially to enter along axle among the present invention makes granules of catalyst be transformed into the small scale backflow of total cross section from the big scale backflow of limit wall, because axial flow velocity upwards carries limit wall catalyzer, tangential flow velocity then utilizes mass force to push catalyzer to central section, and the upward axis of limit wall to flow damage circulate structure, increased the homogeneity of back-mixing, make the Gas-solid Two-phase Flow in the conventional upstriker conversion zone approach plug flow.Beyond all doubt, this has strengthened the mixing efficiency that oil gas contacts with granules of catalyst.
2. three sections reaction zones dividing along the riser tube bed height have been adopted among the present invention, by conditioned reaction intensity, suppress the technical measures that reaction takes place to pay intermediate product, comprise the new cold shock of the residence time, employing in the control differential responses district with medium etc., reach the purpose of voluminous low-carbon (LC) isomeric olefine or propylene.
3. the present invention had all adopted this special measure of radial shrinkage before first reaction zone and second reaction zone, promoted gas together with part and was tangentially entered by axle, and the symphyogenetic result of this two measure is downward landing and the back-mixing that has prevented the top catalyzer effectively.
4. adopted special continuous gas-solid separating device among the present invention, lighter hydrocarbons are drawn in the autoreaction district as early as possible, avoid and reduced and crossed the generations that reaction is paid in cracking, thermally splitting and hydrogen transference etc., guaranteed that high olefin degree in gas and the gasoline product and the high olefin in the isomeric olefine are to the alkane ratio.
5. the inventive method improves 2 times than the isomeric olefine productive rate of normal flow fluidized catalytic cracking under the same conditions, and productivity of propylene improves 2～3 times,
Fig. 1 is the riser tube reactive system synoptic diagram that has improved provided by the invention.
Number being described as follows of [1]～[20] among the figure: [1] is pre lift zone; [2] be first reaction zone; [3] be second reaction zone; [4] be the 3rd reaction zone; [5] once enter inclined tube for regenerator; [6] be the gaseous media inlet; [7] be the bottom gas distributor; [8] be that [9] are a feed nozzle along the tangential gaseous media nozzle of axle, [10] are the second reaction zone bottom; [11] enter inclined tube for the regenerator secondary; [12] be along the tangential gaseous media nozzle of axle; [13] be the secondary feeds nozzle; [14] be the liquid medium inlet; [15] be the descending bed of gas solid separation; [16] be stripping stage; [17] be bell-type porous gas solid separation structure; [18] be the enclosed cyclonic separator; [19] be that the excessive part [20] of riser reactor radial shrinkage is the inlet tube of cyclonic separator.
Fig. 2 is a bell-type porous isolating construction synoptic diagram provided by the invention.
To give further instruction to the present invention by example below, but not thereby limiting the invention.
Used catalyzer is a kind of semi-synthetic carried catalyst that contains y-type zeolite and pentasil type zeolite that is used for fluid catalytic cracking in the example, its industrial trade mark is RFC (Qilu Petrochemical company catalyst plant Industrial products), before using through 790 ℃ of burin-in process of 100% water vapor 8 hours.
Example 1
This example explanation on the medium-sized riser arrangement of having improved provided by the invention, when being raw material with paraffinic base mixing heavy oil, the performance of voluminous low-carbon (LC) isomeric olefine provided by the invention and producing more propylene process.
Used stock oil specification performance is listed in table 1.Result of implementation gained data are listed in table 2.For the purpose of contrast, same catalyst on the medium-sized riser arrangement of routine routinely the FCC mode result that operates gained also one be listed in table 2.
By table 2 data as can be known: processing method provided by the invention productive rate of low-carbon (LC) isomeric olefine and propylene on the specific device of the present invention all can be much higher than FCC.
Table 1 boiling range, ℃ initial boiling point 249; 60%522 characterization factors, 12.4 density (20 ℃), g/cm
30.8687 kinematic viscosity, mm
2/ s 14.82 (80 ℃); (9.334 100 ℃) zero pour, ℃ 36 carbon residues, heavy % 1.8 carbon/hydrogen (weight ratio) 6.44 sulphur, heavy % 0.11 nitrogen, heavy % 0.15 basic nitrogen, ppm 581 iron, ppm 2.5 nickel, ppm 2.1 vanadium, ppm＜0.1 sodium, ppm 2.6 colloids, heavy % 11.2 bituminous matters, heavy % 0.2
Table 2
| Purpose | Fecund i-C = | Fecund C3 = | ????FCC |
| Operating gear | The present invention | The present invention | Conventional FCC |
| Temperature of reaction, ℃ total residence time, second is a district wherein, second two districts, second three districts, second | ????530 ????1.7 ????0.5 ????0.7 ????0.5 | ????530 ????3.0 ????0.5 ????1.5 ????1.0 | ????530 ????3.8 ?????- ?????- ?????- |
| Transformation efficiency, heavy % C 3 =iC 4 =iC 5 =iC 4 =+iC 5 = | ????83.33 ????10.39 ????5.93 ????7.20 ????13.13 | ????83.33 ????12.87 ????5.12 ????6.74 ????11.86 | ????71.37 ????8.14 ????3.68 ????5.14 ????8.82 |
| iC 4 =/∑C 4 =iC 5 =/∑C 5 =iC 4 =/∑C 4° | ????0.42 ????0.69 ????1.65 | ????0.36 ????0.65 ????1.19 | ????0.39 ????0.69 ????1.01 |
Example 2
This example further specifies the result that voluminous low-carbon (LC) isomeric olefine provided by the invention and producing more propylene process are implemented on full scale plant.
Raw materials used fuel oil meter lattice performance is listed in table 3.Result of implementation gained data are listed in table 4.For the purpose of contrast, same catalyst FCC operation gained result routinely also one is listed in table 4.
Table 3 boiling range, ℃ initial boiling point 233; 70%500 density (20 ℃), g/cm
30.8809 kinematic viscosity, mm
2/ s 13.5 (80 ℃); (8.09 100 ℃) zero pour, ℃ 40 carbon residues, heavy % 3.2 carbon/hydrogen (weight ratio) 6.63 sulphur, heavy % 0.33 nitrogen, heavy % 0.08 basic nitrogen, ppm 600 iron, ppm 5.95 nickel, ppm 3.73 vanadium, ppm 11.52 bronze medals, ppm 0.12 colloid, heavy % 12.4 bituminous matters, heavy % 0.9
Table 4
| Operating gear | The present invention | The present invention | Conventional FCC |
| Temperature of reaction, ℃ agent-oil ratio, total residence time, second is a district wherein, second two districts, second three districts, second | ????530 ????9.8 ????1.8 ????0.5 ????0.8 ????0.5 | ????530 ????9.5 ????3.5 ????0.5 ????1.5 ????1.5 | ????510 ????5.5 ????4.0 ?????- ?????- ?????- |
| Conversion ratio; Heavy % material balance, the wherein dry gas liquefied gas gasoline, diesel heavy oil coke loss of heavy % cracked gas | ????81.64 ????34.00 ????2.63 ????31.37 ????42.03 ????14.07 ????4.29 ????5.21 ????0.40 | ????81.87 ????33.23 ????3.51 ????29.72 ????39.58 ????18.13 ????0.00 ????7.68 ????0.44 | ????75.64 ????29.90 ????2.53 ????27.37 ????38.94 ????17.46 ????7.90 ????6.35 ????0.45 |
| Wherein olefins yield weighs % C 3 =iC 4 =iC 5 =iC 4 =+iC 5 =C 3 =+iC 4 =+iC 5 = | ????8.26 ????5.58 ????5.73 ????11.31 ????19.57 | ????10.23 ????4.82 ????5.36 ????10.18 ????20.41 | ????8.9 ????3.2 ????4.6 ????7.8 ????16.7 |
Claims (10)
1. the fluidized catalytic cracking method of a voluminous low-carbon (LC) isomeric olefine is characterized in that:
One by pre lift zone [1] and three sections reaction zones [2,3,4] in the riser reactor of Gou Chenging, the partial regeneration agent is respectively via the bottom with after twice lifting of the gaseous media that tangentially enters, with mix by a charging oil gas that radially sprays into and enter radial shrinkage immediately first reaction zone, after 0.5～1.0 second the residence time, enter radially the second reaction zone bottom of having expanded than first reaction zone.At this position, the lifting of the gaseous media of another part regenerator through tangentially entering along axle, with mix by the secondary feeds oil gas that radially sprays into and from the logistics of first reaction zone after enter radial shrinkage immediately second reaction zone, after 0.5～1.0 second the residence time, enter the 3rd reaction zone that is positioned at the riser tube horizontal section, and the cold shock medium is injected wherein.Logistics is 0.5～1.0 second in the 3rd reaction zone to the residence time that exports the position, and the total residence time in the riser tube reactive system is 1.0～2.0 seconds.Educt flow after the cold shock enters one to have the separation system that the descending bed of continuous multi-stage gas solid separation structure forms by enclosed cyclonic separator and and carries out gas solid separation, isolated gas phase is drawn by the outlet of cyclonic separator, and granules of catalyst enters revivifier through stripping.
2. in accordance with the method for claim 1, it is characterized in that the wherein said regenerator that enters first reaction zone accounts for regenerator circulation total amount below 50%; The regenerator that is entered by the second reaction zone bottom accounts for regenerator circulation total amount more than 50%.
3. in accordance with the method for claim 1, it is characterized in that whole heavy component with the small part relative mixture than light constituent of a wherein said charging for desiring to mix as reaction raw materials, inlet amount accounts for below 60% of total feed; Secondary feeds be major part as reaction raw materials than light constituent, inlet amount accounts for more than 40% of total feed.
4. the fluidized catalytic cracking method of a producing more propylene is characterized in that:
One by pre lift zone [1] and three sections reaction zones [2,3,4] in the riser reactor of Gou Chenging, the partial regeneration agent is respectively via the bottom with after twice lifting of the gaseous media that tangentially enters, with mix by a charging oil gas that radially sprays into and enter radial shrinkage immediately first reaction zone, after 0.5～1.0 second the residence time, enter radially the second reaction zone bottom of having expanded than first reaction zone.At this position, the lifting of the gaseous media of another part regenerator through tangentially entering along axle, with mix by the secondary feeds oil gas that radially sprays into and from the logistics of first reaction zone after enter radial shrinkage immediately second reaction zone, after 1.0～1.5 seconds the residence time, enter the 3rd reaction zone that is positioned at the riser tube horizontal section, and the cold shock medium is injected wherein.Logistics is 0.5～1.0 second in the 3rd reaction zone to the residence time that exports the position, and the total residence time in the riser tube reactive system is 2.0～4.5 seconds.Educt flow after the cold shock enters one to have the separation system that the descending bed of continuous multi-stage gas solid separation structure forms by enclosed cyclonic separator and and carries out gas solid separation, isolated gas phase is drawn by the outlet of cyclonic separator, and granules of catalyst enters revivifier through stripping.
5. in accordance with the method for claim 4, it is characterized in that the wherein said regenerator that enters first reaction zone accounts for regenerator circulation total amount more than 50%; The regenerator that is entered by the second reaction zone bottom accounts for regenerator circulation total amount below 50%.
6. in accordance with the method for claim 4, it is characterized in that the heavy component and relative mixture than light constituent of a wherein said charging for desiring to mix as reaction raw materials, inlet amount accounts for more than 40% of total feed; Secondary feeds is a remaining heavy component and than the mixture of light constituent, and inlet amount accounts for below 60% of total feed.
An improvement that is used for claim 1 or 4 methods the riser tube reactive system, it is characterized by this system and form: the riser reactor that (1) is made of pre lift zone and first, second and third reaction zone of dividing along bed height by following two portions; (2) the gas-solid Quick Separation System that constitutes by the descending bed and the enclosed cyclonic separator of the bell-type porous gas solid separation structure that contains multistage, its structure is as follows:
Be provided with regenerator inlet inclined tube [5], the gas distributor [7] that communicates with gaseous media inlet [6], along being the excessive part [19] of a radial shrinkage between the pre lift zone [1] of a tangential gaseous media nozzle [8] of axle and a feed nozzle [9] and first reaction zone [2] that is positioned at above it, first reaction zone and be positioned at its top second reaction zone [3] between for radial dilatation, be provided with regenerator inlet inclined tube [11], along a tangential gaseous media nozzle [12] and the second reaction zone bottom [10] of secondary feeds nozzle [13], second reaction zone top is to be positioned at the riser tube horizontal section, the end points place is provided with the 3rd reaction zone [4] of liquid medium inlet [14], its outlet is connecting descending bed [15], the inlet tube [20] of enclosed cyclonic separator [18] extends in this descending bed, is the placed in-line bell-type porous of the multistage gas solid separation structure [17] that fuses with it under this extension.
8. according to the described reactive system of claim 7, it is characterized in that in the said riser reactor along tangential gaseous media nozzle [8] or [12] of axle being 2～8, along the perisporium uniform distribution, nozzle opening up, axial angle is 20～40 °.
9. according to the described reactive system of claim 7, it is characterized in that the contraction or the flare angle of radial shrinkage in the said riser reactor or expansion is 45～80 °.
10. according to the described reactive system of claim 7, it is characterized in that the placed in-line bell-type porous of said multistage gas solid separation structure is to be in series with the hood configuration that the cover that is connected thereon constitutes by pipe core by 4～10 sections, this pipe core is coaxial with the footpath with inlet tube [20], have equally distributed 3～9 apertures of 1～3 row at cover lower edge pipe core perisporium, total hole area is 0.3～1.2 times of inlet tube [20] sectional area on the multistage hood configuration, angle α between cover and pipe core is 15～45 °, the height H of cover is 3～10 times of hole diameter, and the height h of no angle vertical section is about 1/2nd of cover height H on the cover.
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| CN97120272A CN1058046C (en) | 1997-11-11 | 1997-11-11 | Catalyst cracking method for producing in high-yield olefin and lift-leg reaction system thereof |
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| CN97120272A CN1058046C (en) | 1997-11-11 | 1997-11-11 | Catalyst cracking method for producing in high-yield olefin and lift-leg reaction system thereof |
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| US4871446A (en) * | 1986-09-03 | 1989-10-03 | Mobil Oil Corporation | Catalytic cracking process employing mixed catalyst system |
| EP0259156A1 (en) * | 1986-09-03 | 1988-03-09 | Mobil Oil Corporation | Process for fluidized catalytic cracking with reactive fragments |
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