CN1137968C - Two-stage catalytic cracking process for hydrocarbon oil - Google Patents
Two-stage catalytic cracking process for hydrocarbon oil Download PDFInfo
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- CN1137968C CN1137968C CNB001228455A CN00122845A CN1137968C CN 1137968 C CN1137968 C CN 1137968C CN B001228455 A CNB001228455 A CN B001228455A CN 00122845 A CN00122845 A CN 00122845A CN 1137968 C CN1137968 C CN 1137968C
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Abstract
The present invention relates to a two-stage catalytic cracking method of hydrocarbon oil, which comprises: the hydrocarbon oil firstly contacts a cracking catalyst in a first reactor and reacts with the cracking catalyst, generated oil gas is conveyed into a second reactor to contact a catalyst containing five-membered ring high-silicon zeolite and to react with the catalyst containing five-membered ring high-silicon zeolite, and generated oil gas is conveyed into a fractionating tower and separated. The catalysts with deposited carbon, which are in the first reactor and the second reactor, are respectively stripped with steam and regenerated, and the regenerated catalysts are circularly used. The method has the characteristics of high conversion capability of heavy oil, high product selectivity, etc. The method comprises economic hydrocarbon processing course.
Description
The invention belongs to the catalyst cracking method of hydrocarbon ils under the situation that does not have hydrogen, more particularly, is a kind of improved two-stage catalytic cracking process.
In the catalytic cracking process of routine, the steam atomizing of stock oil water also sprays in the riser tube, contacts with high temperature catalyst (600～700 ℃) from revivifier therein, vaporizes immediately and reacts.The residence time of oil gas in riser tube is very short, generally has only several seconds.Reaction product is isolated through cyclonic separator and is left reactor behind the catalyzer of carrying secretly and remove separation column.Long-pending have the catalyzer (title reclaimable catalyst) of coke to fall into following stripping stage by settling vessel.The chevron shaped plate washer of multilayer is housed in the stripping stage and feeds overheated steam in the bottom, oil gas that adsorbs on the reclaimable catalyst and the oil gas between the particle are displaced by water vapour and return top.Reclaimable catalyst behind stripping enters revivifier by inclined tube to be generated.The main effect of revivifier is the carbon deposit that generates because of reaction on the burning-off catalyzer, activity of such catalysts is recovered.Catalyzer after the regeneration (title regenerator) falls into upflow tube, sends reactor cycles back to through regenerator sloped tube and uses.
On the basis of above-mentioned catalyst cracking method, disclosed a kind of catalyst cracking method of two reactor among the ZL94217873.4.Concentrate in the 7th nd Annual Meeting of catalytic cracking cooperative groups, name is called the paper of " adopt two-stage riser FCC technology fortifying catalytic reaction process, reduce content of olefin in gasoline research " and has also reported this method.This method is with the two-stage riser reactors in series, and stock oil at first contacts with the high temperature regeneration agent in first section reactor and reacts, and the reaction times should be less than 1 second, and reacted oil gas separates immediately with catalyzer.The reaction oil gas of being told injects second section reactor, contacts, reacts with the agent of new regenerated high temperature regeneration once more, makes oil gas and catalyst separating in experience after the short reaction times equally, and reaction oil gas is sent into and carried out product separation in the subsequent separation system.Long-pendingly have the spent agent of coke to send into the revivifier coke burning regeneration behind stripping by first section reactor and second section reactor are isolated, the catalyzer after the regeneration returns in first section and second section reactor and recycles.Adopt this two-stage catalytic cracking process, because the average activity and the selectivity of catalyzer improve greatly, shortened the reaction times, thereby strengthened catalyzed reaction, reduce thermal response and disadvantageous secondary reaction effectively, can reach the purpose that improves reaction depth, improves product distribution and quality product.
On the basis of above-mentioned two-stage catalytic cracking process, the purpose of this invention is to provide a kind of two-stage catalytic cracking process that has improved, distribute and quality product with the further product that improves.
Hydrocarbon oil catalytic cracking method provided by the invention may further comprise the steps: the hydrocarbon raw material after (1) preheating contacts with cracking catalyst in first reactor, and under the catalytic cracking reaction condition, react, contact separated after 0.5～1.0 second reaction oil gas immediately with cracking catalyst, isolated oil gas is sent into second reactor, the cracking catalyst of carbon deposit is sent into first revivifier, coke burning regeneration under the effect of oxygen-containing gas, the catalyzer after the regeneration return first reactor cycles and use; (2) contact with the catalyzer that contains the five-ring supersiliceous zeolite different in second reactor from the oil gas of first reactor and react with step (1), 350～500 ℃ of temperature of reaction, catalyzer is 4～30 with weight ratio from the oil gas of first reactor, reaction pressure is 0.1～0.34MPa, reaction times is 2.0～4.0 seconds, the separating reaction oil gas and the catalyzer of carbon deposit, isolated oil gas is sent into separation column and is carried out product separation, the catalyzer of carbon deposit is sent into second revivifier behind stripping, coke burning regeneration under the effect of oxygen-containing gas, the catalyzer after the regeneration return second reactor cycles and use.
Now hydrocarbon oil catalytic cracking method provided by the invention is described in detail as follows:
The hydrocarbon raw material that the present invention was suitable for is conventional catalytically cracked stock, and it can be selected from: the mixture of one or more in normal pressure wax oil, long residuum, vacuum residuum, wax tailings, deasphalted oil, hydrocracking tail oil or other secondary processing fraction oil.
In method provided by the invention, first reactor can be the reactor that is suitable for any pattern of catalytic cracking process, for example, riser reactor, fluidized-bed reactor, down-flow reactor, moment contact reactor etc.
The cracking catalyst that contacts with hydrocarbon raw material in first reactor is the solid acid catalyst that is applicable to catalytic cracking process, its active ingredient is a catalytic cracking catalyst multiple zeolite commonly used, comprise the modified product that X type zeolite, y-type zeolite, mordenite, β zeolite and they obtain after ion-exchange or various physical chemistry method are handled, as USY, REY, REHY, HZSM-5, RE-ZSM-5 etc.The catalyzer that cracking catalyst described here can be among the CN1072203A to be adopted, the catalyzer that also can be among the CN1085885A to be adopted.
Hydrocarbon raw material in first reactor with regeneration after cracking catalyst contact, utilize the pyritous cracking catalyst to make the hydrocarbon raw material instant vaporization, and react under following condition: temperature of reaction is 490～650 ℃, the weight ratio of cracking catalyst and hydrocarbon raw material is 3～30, reaction times is 0.5～1.0 second, and reaction pressure is 0.2～0.34MPa.Reaction oil gas in first reactor and catalyzer need in time be drawn, and sharp separation, and isolated oil gas is sent into second reactor and continued reaction.Have the cracking catalyst of coke to send into first revivifier and amass, coke burning regeneration under the effect of oxygen-containing gas, the regeneration condition of cracking catalyst are 670～750 ℃ of dense-phase bed temperature, and regeneration pressure is 0.26～0.34MPa.First revivifier can be selected catalytic cracking process revivifier pattern commonly used for use, for example, and single hop regeneration, two-stage regeneration, fast bed regeneration etc.
In method provided by the invention, enter second reactor from the oil gas of first reactor.Described second reactor can be selected riser reactor and/or fluidized-bed reactor for use.In second reactor, with catalyzer from the contact of the oil gas of first reactor be with first reactor in the different solid acid catalyst that contains the five-ring supersiliceous zeolite of cracking catalyst.Described five-ring supersiliceous zeolite can be the H type, also can be the zeolite through rare earth, phosphorus, zinc or gallium modification.In addition, can also contain in other catalytic cracking catalyst zeolite commonly used one or more in this catalyzer, the modified product that obtains after ion-exchange or various physical chemistry method are handled of X type zeolite, y-type zeolite, mordenite, β zeolite and they for example is as USY, REY, REHY etc.The catalyzer that is used for second reactor described here can be the catalyzer described in the CN1085825A, also can be the catalyzer described in the CN1072201A.
Enter second reactor from the oil gas in first reactor, contact with the catalyzer that contains the five-ring supersiliceous zeolite different after the regeneration with step (1) catalyst system therefor, and under following condition, react: 350～500 ℃ of temperature of reaction, reaction pressure is 0.1～0.34MPa, the weight ratio of catalyzer and reaction oil gas is 4～30, and the reaction times is 2.0～4.0 seconds.In second reactor, finish the oil gas of reaction process and the catalyzer of carbon deposit need in time by drawing in the reactor and sharp separation.Isolated oil gas is sent into and is carried out product separation in the separation column.The catalyzer of carbon deposit enters second revivifier, coke burning regeneration under the effect of oxygen-containing gas.The operational condition of second revivifier is: 550～600 ℃ of regeneration dense-phase bed temperature, regeneration pressure 0.2～0.34MPa.Catalyzer after the regeneration returns second reactor cycles and uses.In method provided by the invention, when step (2) adopts lower temperature of reaction, for example 350 ℃, can earlier the catalyzer appropriateness that contains the five-ring supersiliceous zeolite after the regeneration be cooled off, and then return second reactor cycles and use.Second revivifier can be selected catalytic cracking process revivifier pattern commonly used for use, for example, and single hop regeneration, two-stage regeneration, fast bed regeneration etc.
Below in conjunction with accompanying drawing method provided by the invention is given further instruction, but not thereby limiting the invention.
As shown in Figure 1, in first reactor 2, hydrocarbon raw material 6 with contact from the cracking catalyst after the regeneration of first revivifier 1 and react, the long-pending catalyzer that coke is arranged after separating reaction oil gas and the reaction, isolated oil gas is sent into and is continued reaction in second reactor 4, and the catalyzer of carbon deposit in stripper 3 with superheated vapour 8 counter current contact of injecting by stripper bottom, with between the displacement granules of catalyst and the entrained oil gas of granule interior.Catalyzer behind the stripping is sent into first revivifier 1, coke burning regeneration under the effect of air.Regeneration air 7 is entered by the bottom of first revivifier.Catalyzer after the regeneration returns first reactor cycles and uses.
After entering second reactor 4 from the oil gas of first reactor 2, contact with the catalyzer that contains the five-ring supersiliceous zeolite and react.The oil gas behind the separating reaction and the catalyzer of carbon deposit, isolated oil gas is sent into separation column through pipeline 9 and is carried out product separation.And the catalyzer of carbon deposit is sent into behind the water vapor stripping in second revivifier 5, coke burning regeneration under the effect of air.Regeneration air 7 is entered by the bottom of second revivifier.Catalyzer after the regeneration returns second reactor cycles and uses.
Compared with prior art, the characteristics of hydrocarbon oil catalytic cracking method provided by the invention are mainly reflected in the following aspects:
At first, the present invention organically combines two cover reaction-regeneration systems by reaction oil gas in the hydrocarbon oil catalytic cracking reaction process, and this technical scheme is that favourable condition has been created in the optimization of catalytic cracking reaction process.For example, can regulate the reaction conditions of hydrocarbon ils in each reactor neatly, to improve the productive rate and the quality of high-value products such as vapour, diesel oil according to the needs of purpose product.
In addition, the catalyzer that hydrocarbon ils is contacted in two reactors is to form and the distinct two kinds of catalyzer of character, and described catalyzer all is just to have passed through regenerated to have greater activity and catalyzer optionally.Therefore, can the catalytic cracking reaction of hydrocarbon ils be carried out towards our desirable direction by reasonably selecting catalyzer for use.In first reactor, select the strong catalyzer of heavy oil cracking ability for use, make more macromole petroleum hydrocarbon be converted into petroleum products; And selected catalyzer should have selectivity hydrogen transference preferably, isomerization and aromatization performance in second reactor, and the quality of vapour, diesel product is improved in this reactor.
Because the present invention is accomplished the lighting of heavy oil and the improvement of oil quality by the improvement to the hydrocarbon oil catalytic cracking method in same reaction process, therefore, from the whole process of refining of petroleum, the present invention can save energy consumption, material consumption, is a kind of hydrocarbon processing method of less expensive.
Fig. 1 is a schematic flow sheet of the present invention.
The following examples will give further instruction to the present invention, but not thereby limiting the invention.Adopt the raw material oil properties to see Table 1 in the process of the test, the character of catalyzer sees Table 2, and wherein the RHZ-300 catalyzer contains REHY type zeolite, industrial by Qilu Petrochemical company catalyst plant; The GOR-C catalyzer contains ZRP zeolite, industrial by Ba Ling company Chang Ling catalyst plant.
Embodiment
Present embodiment explanation: adopt hydrocarbon oil catalytic cracking method provided by the present invention to handle heavy petroleum hydrocarbon, can obtain comparatively that the ideal product distributes, and the character of vapour, diesel product is better than conventional heavy oil catalytic cracking process.
Stock oil and the catalyzer in the table 2 in the employing table 1 are tested on the catalytic cracking middle-scale device.Testing sequence is summarized as follows: inject first reactor (riser reactor) about fuel oil preheating to 250 ℃, after steam atomizing, contact and react with the RHZ-300 catalyzer after the regeneration, temperature of reaction is that the weight ratio (agent-oil ratio) of 520 ℃, catalyzer and stock oil is 8.0, the reaction times is 1.0 seconds, the oil gas behind the separating reaction and the catalyzer of carbon deposit.Reaction oil gas is sent in second reactor (riser reactor) through pipeline.The RHZ-300 catalyzer of carbon deposit is sent into first revivifier behind stripping.Feed the pressurized air after the heating in first revivifier, the regeneration dense phase temperature is that 706 ℃, regeneration pressure are 0.22MPa, and the catalyzer after the regeneration returns first reactor cycles and uses.In second reactor, contact and react from the oil gas of first reactor with GOR-C catalyzer after the regeneration, temperature of reaction is 465 ℃, the weight ratio of catalyzer and reaction oil gas is 14.5, reaction times is 2.0 seconds, the oil gas behind the separating reaction and the catalyzer of carbon deposit, the oil gas of being told is sent in the separation column, further is separated into various products, and the catalyzer of carbon deposit is sent into coke burning regeneration in second revivifier behind stripping.Feed the pressurized air after the heating in second revivifier, the regeneration dense phase temperature is that 560 ℃, regeneration pressure are 0.22Mpa, and the catalyzer after the regeneration returns second reactor cycles and uses.
The principal reaction condition is referring to table 3, and material balance data sees Table 4, and the main character of gasoline products sees Table 5, and the main character of diesel product sees Table 6.
Comparative Examples
This Comparative Examples is heavy raw oil shown in the employing table 1 and refinery catalyst for heavy oil catalytic cracking RHZ-300 commonly used, tests on the riser tube middle-scale device.
Testing sequence is summarized as follows: injecting lift pipe reactor bottom about fuel oil preheating to 250 ℃, after steam atomizing, contact and react with the RHZ-300 catalyzer after the regeneration, temperature of reaction is that 520 ℃, agent-oil ratio are 8.0, the reaction times is 3.0 seconds, the separating reaction oil gas and the catalyzer of carbon deposit.Reaction oil gas is sent into through pipeline and further is separated into various products in the separation column.The catalyzer of carbon deposit is sent into coke burning regeneration in the revivifier behind stripping.The regeneration dense phase temperature is that 705 ℃, regeneration pressure are 0.22MPa, and the catalyzer Returning reactor after the regeneration recycles.
The principal reaction condition sees Table 3, and material balance sees Table 4, and gasoline products character sees Table 5, and diesel product character sees Table 6.
The reaction result of embodiment and Comparative Examples is compared as can be seen, and hydrocarbon oil catalytic cracking method provided by the present invention has stronger heavy oil conversion performance and better products selectivity, and the quality of vapour, diesel product be improved significantly.Table 1
Table 2
Table 3
Table 4
Table 5
Table 6
| Density (20 ℃), kilogram/rice 3 | 905.0 |
| Kinematic viscosity (100 ℃), millimeter 2/ second | 48.29 |
| Zero pour, ℃ | 35 |
| Carbon residue, heavy % | 4.78 |
| Sulphur content, heavy % | 0.11 |
| Nitrogen content, heavy % | 0.24 |
| Carbon content, heavy % | 86.5 |
| Hydrogen richness, heavy % | 12.94 |
| Heavy metal content, ppm | |
| Nickel | 4.6 |
| Iron | 3.7 |
| Copper | 0.03 |
| Vanadium | 0.01 |
| Boiling range, ℃ | |
| Initial boiling point | 345 |
| 5％ | 453 |
| 10％ | 492 |
| 30％ | / |
| 50％ | / |
| 500 ℃ distillate v% | 29.0 |
| The catalyzer title | RHZ-300 | GOR-C |
| Chemical constitution, heavy % | ||
| Aluminum oxide | 54.2 | 48.7 |
| Sodium oxide | 0.03 | 0.12 |
| Apparent density, kilogram/rice 3 | 860 | 750 |
| Pore volume, milliliter/gram | 0.26 | 0.36 |
| Specific surface area, rice 2/ gram | 160 | 256 |
| Abrasion index, %/hour | 1.2 | 2.2 |
| Micro-activity (800 ℃ of 4h) | 73.0 | 79.1 |
| Size composition, heavy % | ||
| ＜20 microns | 3.1 | 4.6 |
| 20～40 microns | 21.1 | 14.6 |
| 40～80 microns | 55.5 | / |
| 80～110 microns | 13.8 | / |
| ＞110 microns | 6.5 | / |
| The hydrothermal aging condition: | 800℃、17h、100％H 2O | |
| Aging back micro-activity | 63 | 70 |
| The principal reaction condition: | Comparative Examples | Embodiment |
| First reactor: pressure (cutting off), MPa | 0.18 | 0.18 |
| Temperature, ℃ | 520 | 520 |
| Agent-oil ratio | 8.0 | 8.0 |
| Reaction times, s | 3.0 | 1.0 |
| First revivifier: pressure (cutting off), MPa | 0.22 | 0.22 |
| Temperature, ℃ | 705 | 706 |
| Second reactor: pressure (cutting off), MPa | / | 0.20 |
| Temperature, ℃ | / | 465 |
| Agent-oil ratio | / | 14.5 |
| Reaction times, s | / | 2.0 |
| Second revivifier: pressure (cutting off), MPa | / | 0.22 |
| Temperature, ℃ | / | 560 |
| Product distributes, heavy % | Comparative Examples | Embodiment |
| Dry gas | 3.17 | 3.28 |
| Liquefied gas | 15.11 | 15.90 |
| Gasoline | 39.18 | 39.53 |
| Diesel oil | 28.84 | 27.93 |
| Slurry oil | 4.08 | 3.54 |
| Coke | 9.09 | 9.30 |
| Loss | 0.53 | 0.52 |
| Add up to | 100.00 | 100.00 |
| Gasoline property | Comparative Examples | Embodiment |
| Density (20 ℃), kilogram/rice 3 | 718.6 | 721.3 |
| Octane value | ||
| RON | 89.6 | 90.5 |
| MON | 79.6 | 80.4 |
| Inductive phase, minute | 266 | 555 |
| Existent gum, milligram/100 milliliters | ＜2.0 | ＜2.0 |
| Sulphur content, ppm | 121 | 102 |
| Nitrogen content, ppm | 56 | 53 |
| Group composition, heavy % | ||
| Stable hydrocarbon | 34.97 | 46.00 |
| Alkene | 42.89 | 27.68 |
| Aromatic hydrocarbon | 22.14 | 26.32 |
| Boiling range, ℃ | ||
| Initial boiling point | 39 | 40 |
| 10％ | 56 | 57 |
| 50％ | 97 | 99 |
| 90％ | 175 | 177 |
| Do | 199 | 198 |
| Diesel oil character | Comparative Examples | Embodiment |
| Density (20 ℃) kilogram/rice 3 | 869.8 | 870.2 |
| Zero pour ℃ | -12.0 | -13.0 |
| Existent gum, milligram/100 milliliters | 241.0 | 234.0 |
| Sulphur content, ppm | 321 | 318 |
| Basic nitrogen, ppm | 146 | 142 |
| Cetane value | 34 | 36 |
| Boiling range, ℃ | ||
| Initial boiling point | 201 | 200 |
| 10％ | 224 | 225 |
| 50％ | 269 | 271 |
| 90％ | 331 | 329 |
| Do | 342 | 340 |
Claims (8)
1, a kind of two-stage catalytic cracking process of hydrocarbon ils is characterized in that this method may further comprise the steps:
(1) hydrocarbon raw material after the preheating contacts with cracking catalyst in first reactor, and under the catalytic cracking reaction condition, react, reacted oil gas separates immediately with cracking catalyst, isolated oil gas is sent into second reactor, the cracking catalyst of carbon deposit is sent into first revivifier, coke burning regeneration under the effect of oxygen-containing gas, the catalyzer after the regeneration return first reactor cycles and use; The reaction conditions of described hydrocarbon raw material in first reactor is: temperature of reaction is 490～650 ℃, and the weight ratio of cracking catalyst and hydrocarbon raw material is 3～30, and the reaction times is 0.5～1.0 second, and reaction pressure is 0.2～0.34Mpa;
(2) contact with the catalyzer that contains the five-ring supersiliceous zeolite different in second reactor from the oil gas of first reactor and react with step (1), 350～500 ℃ of temperature of reaction, the weight ratio of catalyzer and reaction oil gas is 4～30, reaction pressure is 0.1～0.34MPa, reaction times is 2.0～4.0 seconds, the separating reaction oil gas and the catalyzer of carbon deposit, isolated oil gas is sent into separation column and is carried out product separation, the catalyzer of carbon deposit is sent into second revivifier behind stripping, coke burning regeneration under the effect of oxygen-containing gas, the catalyzer after the regeneration return second reactor cycles and use.
2, according to the method for claim 1, it is characterized in that described hydrocarbon raw material is selected from: the mixture of one or more in normal pressure wax oil, long residuum, vacuum residuum, wax tailings, deasphalted oil, hydrocracking tail oil or other secondary processing fraction oil.
3,, it is characterized in that described first reactor can be the reactor that is applicable to any pattern of catalytic cracking process according to the method for claim 1.
4, according to the method for claim 3, it is characterized in that described first reactor is selected from: a kind of in riser reactor, fluidized-bed reactor, down-flow reactor, the moment contact reactor.
5, according to the method for claim 1, it is characterized in that described cracking catalyst is the solid acid catalyst that is applicable to catalytic cracking process, its active ingredient is selected from one or more in the catalytic cracking catalyst multiple zeolite commonly used, comprises the modified product that X type zeolite, y-type zeolite, mordenite, β zeolite and they obtain after ion-exchange or various physical chemistry method are handled.
6,, it is characterized in that second reactor described in the step (2) is riser reactor and/or fluidized-bed reactor according to the method for claim 1.
7, according to the method for claim 1, it is characterized in that in the step (2) that the five-ring supersiliceous zeolite that catalyzer contained that contacts with oil gas from first reactor can be the H type, also can be zeolite through rare earth, phosphorus, zinc or gallium modification; Can also contain in the modified product that X type zeolite, y-type zeolite, mordenite, β zeolite or they obtain one or more in this catalyzer after ion-exchange or various physical chemistry method are handled.
8,, it is characterized in that the catalyzer after the regeneration described in the step (2) returns the use of second reactor cycles after cooling according to the method for claim 1.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| US6866771B2 (en) * | 2002-04-18 | 2005-03-15 | Uop Llc | Process and apparatus for upgrading FCC product with additional reactor with catalyst recycle |
| US6974559B2 (en) * | 2003-02-26 | 2005-12-13 | Intercat Equipment, Inc. | Apparatus for metering catalyst in a fluid catalytic cracking catalyst injection system |
| CN101074392B (en) * | 2006-05-18 | 2010-05-12 | 中国石油天然气股份有限公司 | Production method of propene and high-quality gasoline and diesel oil by two-stage catalyzed crack |
| CN101210197B (en) * | 2006-12-29 | 2011-08-10 | 中国石油化工股份有限公司 | Conversion method for hydrocarbon oil |
| CN101457153B (en) * | 2007-12-14 | 2012-07-18 | 中国石油化工股份有限公司 | Hydrocarbon oil conversion method |
| CN102443419B (en) * | 2010-10-13 | 2014-07-02 | 中国石油化工股份有限公司 | Hydrocarbon oil catalytic cracking method and equipment |
| CN102453500A (en) * | 2010-10-21 | 2012-05-16 | 中国石油化工股份有限公司 | Catalytic cracking method and equipment for hydrocarbon oil |
| US9387449B2 (en) | 2010-11-11 | 2016-07-12 | Baozhen Shi | Catalytic cracking method and apparatus |
| CN102827635B (en) | 2011-06-15 | 2014-04-02 | 石宝珍 | Catalytic cracking method and device thereof |
| CN107573967B (en) * | 2016-07-04 | 2019-08-16 | 中国石油化工股份有限公司 | A kind of method for hydrogen cracking producing boat coal |
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