CN104560185B - The catalysis conversion method of aromatic compound gasoline is rich in a kind of production - Google Patents
The catalysis conversion method of aromatic compound gasoline is rich in a kind of production Download PDFInfo
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G69/00—Treatment of hydrocarbon oils by at least one hydrotreatment process and at least one other conversion process
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Abstract
The catalysis conversion method of aromatic compound gasoline is rich in a kind of production, catalytic cracking light cycle oil obtains light fraction and heavy distillat through cutting, wherein heavy distillat obtains hydrogenation heavy distillat through hydrotreatment, light fraction and hydrogenation heavy distillat enter catalytic cracking unit by different spray nozzles layering separately, under catalytic cracking catalyst exists, carry out cracking reaction, reaction product isolated obtains comprising and is rich in the gasoline of aromatic compound, the product of light cycle oil. Heavy distillat layering that the method adopts independent catalytic cracking unit to process after light fraction and the hydrogenation of light cycle oil enter, can optimize to greatest extent and meet the required harsh conditions of light cycle oil different fractions catalytic cracking reaction, thereby farthest produce the catalytic gasoline that is rich in benzene, toluene and dimethylbenzene.
Description
Technical field
The invention belongs to the catalysis conversion method of petroleum hydrocarbon in the situation that not there is not hydrogen, more specificallySaying, is a kind of catalysis of being produced the gasoline that is rich in benzene,toluene,xylene by catalytic cracking light cycle oilMethod for transformation.
Background technology
Along with the development of crude oil heaviness and the rapid growth of market to light-end products demand, in China, doFor the catalytic cracking technology of heavy oil lighting is rapidly developed. But, a fact must facingThe quality that is catalytic cracking diesel oil (or title " light cycle oil ") is but always relatively poor, and density is large,Arene content is high, and Cetane number is low, even be also difficult to reach day by day tight by diesel oil hydrogenation modification technologyThe diesel oil regulation of lattice. How solving catalytic cracking light cycle oil is an increasingly serious problem. To twoToluene is the important source material of polyester industry, right mainly for the production of p-phthalic acid (PTA) or essencePhthalic acid two formicesters (DMT), and then produce polyester (PET) by PTA and DMT. Therefore,Producing paraxylene by catalytic cracking light cycle oil may be a kind of new approach.
US4585545 has disclosed one full catalytic cracking light cycle oil cut has first been carried out to hydrotreatment,The hydrogenated diesel oil obtaining goes catalytic cracking to produce the catalysis conversion method that is rich in mononuclear aromatics gasoline again.
CN1422327A discloses a kind of method of catalytic cracking light cycle oil upgrading, is by with heavyThe light cycle oil that the first catalytic cracking unit that oil is raw material is produced carries out deep hydrogenation, the hydrogenation obtainingRecycle oil enters the second catalytic cracking unit again. On the basis of the method, CN1423689A emphasizesCatalyst in two catalytic cracking units requires the aperture of selecting shape zeolite and about 5-50% containing 50-95%Be more than or equal to the large pore zeolite of about 0.7nm, optionally to improve light olefin productive rate.
CN1466619A discloses a kind of method for transformation of catalytic cracking light cycle oil, is that catalysis is splitChange riser reactor and be divided into two of upstream and downstream reaction zone, wherein mink cell focus injects catchment, itsThe hydrogenation recycle oil that catalytic cracking production light cycle oil obtains after hydrotreatment injects upstream. At thisOn the basis of method, the charging in CN1425054A method middle and lower reaches district is except hydrogenation recycle oil, alsoIncrease naphtha. In the method, not only hydrogen consumption is high, and hydrogenation recycle oil can be tight in upstream reactionGhost image rings the conversion of the mink cell focus in downstream.
Can find from disclosed document above, that processes for catalytic cracking light cycle oil is importantOne of approach is that it is first carried out to hydrotreatment, and then catalytic cracking. It must be noted that, gently followTherefore how no matter whether hydrogenation of ring oil, compares with the large molecule of mink cell focus, and its molecule is little, bond energy is large,The operating parameter of controlling catalytic cracking is one of key of light cycle oil processing. In addition, light cycle oil asFruit carries out hydrogenation, and the operation control of hydrogenation process is also one of key of light cycle oil processing.
Summary of the invention
The object of the invention is to provide on the basis of existing technology a kind of production to be rich in aromatic series chemical combinationThe catalysis conversion method of thing gasoline.
Catalysis conversion method provided by the invention comprises:
(1) catalytic cracking light cycle oil obtains light fraction and heavy distillat through cutting;
(2) the described heavy distillat of step (1) is carried out hydrogenation under hydrogen and hydrotreating catalyst existenceProcessing reaction, reaction condition is hydrogen dividing potential drop 5.0～10.0MPa, 330～450 DEG C of reaction temperatures, volumeAir speed 2～10.0 hours-1, hydrogen to oil volume ratio 400～1600Nm3/m3, reaction product isolated is addedHydrogen heavy distillat;
(3) the described light fraction of step (1), step (2) enter by different spray nozzles layering separatelyRiser reactor carries out catalytic cracking reaction under catalytic cracking catalyst exists, and reaction condition is:600～710 DEG C of reaction temperatures, agent oil quality is than 5～100,1～10 second oil gas time of staying, water vapourWith the weight ratio 0.01～0.5 of raw material, Catalyst Balance Activity is not more than 65, separates catalytic cracking to be generatedCatalyst and reaction oil gas, wherein reaction oil gas is isolated to and comprises the vapour that is rich in aromatic compoundThe product of oil, light cycle oil.
Preferably the method also comprises: the described catalytic cracking catalyst to be generated of step (3) through stripping, againRaw rear gained regeneration catalyzing Cracking catalyst is returned to riser reactor and is recycled.
The described catalytic cracking light cycle oil of step (1) is selected from allocatalysis cracking unit and produces light circulationOil is or/and this method catalytic cracking unit step (3) light cycle oil that produces, preferably allocatalysis crackingDevice the light cycle oil that produces and this method catalytic cracking unit step (3) light cycle oil that produces.
Method provided by the invention is specific as follows:
Catalytic cracking light cycle oil enters independent fractionating column and cuts, and cutting temperature is controlled at250～260 DEG C, preferably cutting temperature is 260 DEG C, obtains respectively not high from top and the bottom of fractionating columnIn the light fraction of this cutting temperature with higher than the heavy distillat of this cutting temperature.
Hydrotreater is removed in described heavy distillat, under hydrogen and hydrogenation catalyst existence, carries out hydrogenation placeReason reaction, hydroprocessing condition is: hydrogen dividing potential drop 5.0～10.0MPa, preferably 5.0～8.0MPa; InsteadAnswer 330～450 DEG C of temperature, preferably 340～380 DEG C; Volume space velocity 2～10.0 hours-1, hydrogen oil volumeThan 400～1600Nm3/m3. Reaction product isolated obtains heating up in a steamer of 260 DEG C of 250 DEG C of preferred > of initial boiling point >Point, or claim hydrogenated diesel oil, hydrogenation heavy distillat. In described hydrogenation heavy distillat, double ring arene content wants≤20Heavy %, the heavy % in preferably≤10.
Described activity of hydrocatalyst metal component be selected from group vib metal and/or group VIII non-Noble metal, carrier is selected from aluminium oxide, silica, amorphous aluminum silicide any one or several. DescribedGroup vib metal is molybdenum or/and tungsten, and group VIII base metal is that nickel is or/and cobalt. Active metal groupDivide the combination of preferred nickel-tungsten, nickel-tungsten-cobalt, nickel-molybdenum or cobalt-molybdenum.
The light fraction of light cycle oil and the hydrogenation heavy distillat obtaining enter independent catalytic cracking unit,Catalytic cracking catalyst carries out cracking reaction under existing, reaction product isolated obtain dry gas, liquefied gas,Gasoline, light cycle oil, slurry oil, coke. The concrete operations condition of catalytic cracking unit is as follows:
Catalytic cracking unit can be isometrical riser reactor or reducing riser reactor. ≤ 260 DEG CLight fraction can mix with the hydrogenation heavy distillat obtaining after together with enter riser reactor, but preferablySeparately enter riser reactor by different spray nozzles separately. Wherein light fraction is from lower floor's spray of riserMouth (upstream) enters, and hydrogenation heavy distillat enters from the upper strata nozzle (downstream) of riser. Upper,The distance of lower floor's nozzle is to control the time of staying of reaction oil gas in two-layer nozzle distance as 0.01～3Be advisable second, preferably 0.05～1 second. The advantage that light fraction and hydrogenation heavy distillat layering enter is to optimizeMeet the reaction condition of different fractions catalytic cracking, transform thereby realize farthest.
The reaction condition of catalytic cracking unit is: reaction temperature is 600～710 DEG C, preferably 600～680 DEG C;Agent oil quality is than 5～100, and preferably 8～50; 1～10 second oil gas time of staying, preferably 2～8 seconds; PressPower (absolute pressure) 0.15～0.4MPa; The weight ratio of water vapour and raw material is 0.01～0.5 preferred0.02～0.2; Poising agent activity (MAT)≤65.
Catalytic cracking catalyst comprises zeolite, inorganic oxide and optional clay. The content of each componentBe respectively: the heavy % of zeolite 10～50, the heavy % of inorganic oxide 5～90, the heavy % of clay 0～70. WhereinActive component be selected from containing or not containing the one of Y, HY, USY or the Beta zeolite of rare earth, two kindsOr multiple.
The invention has the advantages that:
1, catalytic cracking unit light cycle oil is first cut, and wherein hydrogenation is removed in heavy distillat, canReduce to greatest extent hydrogen consumption;
2, adopt independent catalytic cracking unit to process the double distilled after light fraction and the hydrogenation of light cycle oilDivide also layering to enter, can optimize to greatest extent and meet light cycle oil different fractions catalytic cracking reactionRequired harsh conditions, thus the catalytic gasoline that is rich in benzene, toluene and dimethylbenzene farthest produced.
Brief description of the drawings
Fig. 1 is the catalysis conversion method flow process that aromatic compound gasoline is rich in production provided by the inventionSchematic diagram.
Detailed description of the invention
Further illustrate method provided by the present invention below in conjunction with accompanying drawing, but the present invention not therefore andBe subject to any restriction.
Accompanying drawing is catalysis conversion method schematic flow sheet provided by the invention.
Fig. 1 is the schematic flow sheet of preferred forms of the present invention, but does not limit the present invention. EquipmentWith the shape of pipeline, the restriction that size is not subject to accompanying drawing, but determine as the case may be. Each in accompanying drawingNumbering is described as follows:
1,3-5,7,11-14 all represent pipeline; 2 is fractionating device; 6 is diesel hydrotreating unit; 8,9 is catalytic cracking feeding nozzle; 10 is catalytic cracking reaction device.
Below in conjunction with accompanying drawing, preferred forms provided by the present invention is further described.
Catalytic cracking light cycle oil enters fractionating device 2 through pipeline 1 and cuts, and obtains≤260 DEG CLight fraction and the heavy distillat of 260 DEG C of >. The light fraction of wherein≤260 DEG C is through pipeline 3, catalytic crackingLower floor's feed nozzle 8 enters catalytic cracking reaction device 10. And the heavy distillat of 260 DEG C of > is through pipeline 4Enter diesel hydrotreating unit 6, hydrogen is introduced diesel hydrotreating unit 6 through pipeline 5 simultaneously. After hydrogenationProduct hydrogenated diesel oil enters catalytic cracking reaction device 10 through pipeline 7, catalytic cracking upper strata nozzle 9.The light fraction of≤260 DEG C and hydrogenated diesel oil, in catalytic cracking unit 10, are deposited at catalytic cracking catalystUnder carry out catalytic cracking reaction, reaction product isolated obtains being rich in the Gaoxin of benzene,toluene,xyleneAlkane value gasoline is drawn through pipeline 11, another catalytic cracking reaction product light cycle oil through pipeline 12 draw,Entering fractionating device 2 through pipeline 13,14,1 circulates. For simplicity, other products as dry gas,Liquefied gas, slurry oil etc. do not draw in the drawings.
The following examples will be further described the present invention, but not thereby limiting the invention.In embodiment, in hydrotreatment fixed bed reactors, the hydrotreating catalyst business trade mark of filling isRN-32V, the protective agent business trade mark is RG-1, hydrotreating catalyst and protectant admission spaceRatio is 95:5, produces by Sinopec catalyst branch company.
The physico-chemical property of catalyst that in embodiment, comparative example, catalytic cracking unit uses is in table 1, itsThe business trade mark is HAC, and by Sinopec catalyst, branch company produces.
Raw material (catalytic cracking light cycle oil) character using in embodiment, comparative example is listed in table 2.
Embodiment
The present embodiment explanation adopts method provided by the invention, and raw material is first gently circulated through boiling range cuttingOil light fraction and light cycle oil heavy distillat, cut point is 250 DEG C.
Light cycle oil heavy distillat enters medium-sized hydrogenation plant, and the experimental condition of hydrogenation is: hydrogen dividing potential drop8.0MPa; 360 DEG C of average bed reaction temperatures, volume space velocity 2.0 hours-1, hydrogen to oil volume ratio1100Nm3/m3. In hydrogenation heavy distillat, double ring arene content is 9.6 heavy %.
Light cycle oil heavy distillat after light cycle oil light fraction and hydrogenation enters respectively medium-sized catalytic crackingThe upper and lower layer nozzle of riser reaction unit, wherein lower floor's nozzle is entered in light fraction, and hydrogenation double distilled is divided intoUpper strata nozzle. When the distance of upper and lower two-layer nozzle is the stop of reaction oil gas in two-layer nozzle distanceBetween be 0.5 second. The main operating parameters of kitty cracker is: reaction temperature is 610 DEG C;Agent oil quality is than 20; 7 seconds oil gas time of staying; Pressure (absolute pressure) 0.25MPa; Water vapourWith the weight ratio of raw material be 0.06. Device poising agent activity (MAT) is 62.
Comparative example 1
Medium-sized tester is identical with embodiment with catalyst. The boiling range cut point of light cycle oil is sameEmbodiment, just the heavy distillat after light cycle oil light fraction and hydrogenation fills from medium-sized catalytic cracking after mixingLower floor's nozzle of putting enters. The wherein same embodiment of the hydroconversion condition of the heavy distillat of light cycle oil. Medium-sized urgingChange the same embodiment of operating condition of cracking unit.
Comparative example 2
Medium-sized tester is identical with embodiment with catalyst. Light cycle oil cuts without boiling range,Full cut directly removes hydrogenation plant hydrogenation, and the full cut of light cycle oil after hydrogenation directly enters medium-sized catalysis and splitsLower floor's nozzle of gasifying device. The wherein same embodiment of the hydroconversion condition of the full cut of light cycle oil. Medium-sized urgingChange the same embodiment of operating condition of cracking unit.
Catalytic cracking product distributes and hydrogen consumes in table 3.
Contrast comparative example 1 and comparative example 2 can be found, adopt the method for boiling range cutting, in hydrogenation mistakeIn journey, can obviously reduce hydrogen consumption, hydrogen consumption is reduced to 1.43% from 2.1%. Can find, to the greatest extent simultaneouslyPipe product distributes and makes moderate progress, but is not clearly. And comparative example and comparative example 2 canTo find, not only hydrogen consumption is reduced to 1.43% from 2.1%, and product distributes and obviously improves, performanceIn the time of conversion per pass, gasoline yield is increased to 51.2%, wherein benzene, toluene and dimethylbenzene from 45.51%Absolute yield be increased to 25.8% from 17%.
Table 1HAC catalyst property
Table 2 feedstock oil character
| Feedstock oil title | Catalytic cracking light cycle oil |
| Density (20 DEG C), kg/m3 | 948.8 |
| Freezing point, DEG C | -24 |
| Aniline point, DEG C | <30 |
| 10% carbon residue, heavy % | 0.37 |
| Mean molecule quantity | 187 |
| Boiling range, DEG C | |
| Initial boiling point | 190 |
| 5% | 213 |
| 10% | 222 |
| 30% | 247 |
| 50% | 272 |
| 70% | 303 |
| 90% | 348 |
| 95% | 363 |
| The end point of distillation | 369 |
| Mass spectrography quality composition, % | |
| Alkane | 10.7 |
| Total cycloalkane | 4.6 |
| Total aromatic hydrocarbons | 84.7 |
| Mononuclear aromatics | 31.7 |
| Double ring arene | 45.0 |
| Gross mass | 100.0 |
Table 3
| Embodiment 1 | Comparative example 1 | Comparative example 2 | |
| Hydrogen consumption, % | 1.43 | 1.43 | 2.1 |
| Product distributes, heavy % | |||
| Dry gas | 2.1 | 2.3 | 2.61 |
| Liquefied gas | 15.2 | 15.5 | 16.14 |
| Gasoline | 51.2 | 47.8 | 45.51 |
| Benzene | 3.71 | 2.86 | 2.75 |
| Toluene | 18.55 | 14.32 | 13.75 |
| Dimethylbenzene | 28.13 | 21.72 | 20.85 |
| Benzene+toluene+dimethylbenzene | 25.8 | 18.6 | 17.0 |
| Light diesel fuel | 26.7 | 29.4 | 30.47 |
| Heavy oil | 1.2 | 1.4 | 1.48 |
| Coke | 3.6 | 3.6 | 3.79 |
| Add up to | 100.0 | 100.0 | 100.0 |
Claims (16)
1. a catalysis conversion method for aromatic compound gasoline is rich in production, it is characterized in that thisMethod comprises:
(1) catalytic cracking light cycle oil obtains light fraction and heavy distillat through cutting;
(2) the described heavy distillat of step (1) is carried out hydrogenation under hydrogen and hydrotreating catalyst existenceProcessing reaction, reaction condition is hydrogen dividing potential drop 5.0～10.0MPa, 330～450 DEG C of reaction temperatures, volumeAir speed 2～10.0 hours-1, hydrogen to oil volume ratio 400～1600Nm3/m3, reaction product isolated is addedHydrogen heavy distillat;
(3) the described light fraction of step (1), the described hydrogenation heavy distillat of step (2) are passed through not separatelyEnter riser reactor with nozzle layering, under catalytic cracking catalyst exists, carry out Catalytic Cracking Unit of MeasureShould, reaction condition is: 600～710 DEG C of reaction temperatures, agent oil quality is than 5～100, when oil gas stopsBetween 1-10 second, the weight ratio 0.01～0.5 of water vapour and raw material, Catalyst Balance Activity is not more than 65,Separate catalytic cracking catalyst to be generated and reaction oil gas, wherein reaction oil gas is isolated to and comprises and being rich inThe gasoline of aromatic compound, the product of light cycle oil.
2. according to the method for claim 1, it is characterized in that the described light cycle oil of step (3) returnsStep (1).
3. according to the method for claim 1, it is characterized in that the method also comprises: step (3) instituteState catalytic cracking catalyst to be generated gained regeneration catalyzing Cracking catalyst after stripping, regeneration and return to liftingPipe reactor recycles.
4. according to the method for claim 1, it is characterized in that the cutting temperature of described light cycle oil is250～260℃。
5. according to the method for claim 1, it is characterized in that the described hydrotreatment of described step (2)Condition be hydrogen dividing potential drop 5.0～8.0MPa, 340～380 DEG C of reaction temperatures.
6. according to the method for claim 1, it is characterized in that the described hydrotreatment of described step (2)The active metal component of catalyst is selected from group vib metal and/or group VIII base metal, carrierBe selected from aluminium oxide, silica, amorphous aluminum silicide any one or several.
7. according to the method for claim 6, it is characterized in that described group vib metal be molybdenum or/And tungsten, group VIII base metal is that nickel is or/and cobalt.
8. according to the method for claim 6, it is characterized in that described active metal component be selected from nickel-tungsten,The combination of nickel-tungsten-cobalt, nickel-molybdenum or cobalt-molybdenum.
9. according to the method for claim 1, it is characterized in that double ring arene content in hydrogenation heavy distillatBe not more than 20 heavy %.
10. according to the method for claim 9, it is characterized in that double ring arene content in hydrogenation heavy distillatBe not more than 10 heavy %.
11. according to the method for claim 1, it is characterized in that described riser reactor is isometrical carryingRiser reactors or reducing riser reactor.
12. according to the method for claim 1, it is characterized in that the lower floor nozzle of light fraction from riserEnter, and hydrogenation heavy distillat enters from the upper strata nozzle of riser.
13. according to the method for claim 12, it is characterized in that the distance of upper and lower layer nozzle is with controlThe time of staying of reaction oil gas processed in two-layer nozzle distance is 0.01～3 second.
14. according to the method for claim 13, it is characterized in that the distance of upper and lower layer nozzle is with controlThe time of staying of reaction oil gas processed in two-layer nozzle distance is 0.05～1 second.
15. according to the method for claim 1, it is characterized in that the reaction condition of catalytic cracking unit is:Reaction temperature is 600～680 DEG C, and agent oil quality is than 8～50,2～8 seconds oil gas time of staying, water vapourWith the weight ratio of raw material be 0.02～0.2.
16. according to the method for claim 1, it is characterized in that the described catalytic cracking of step (3) urgesAgent comprises zeolite, inorganic oxide and optional clay, and the content of each component is respectively: zeolite10～50 heavy %, the heavy % of inorganic oxide 5～90, the heavy % of clay 0～70, wherein active component is choosingSelf-contained or not containing the one of Y, HY, USY or the Beta zeolite of rare earth, two or more.
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| CN109423335B (en) * | 2017-08-30 | 2021-07-09 | 中国石油化工股份有限公司 | Catalytic cracking method for increasing gasoline yield |
| CN109554193B (en) * | 2017-09-26 | 2021-02-09 | 中国石油化工股份有限公司 | Catalytic cracking method for increasing production of low-olefin and high-octane gasoline |
| CN110551526B (en) * | 2018-05-30 | 2021-08-06 | 中国石油化工股份有限公司 | Processing method of catalytic cracking light cycle oil |
| CN110551527B (en) * | 2018-05-30 | 2021-08-06 | 中国石油化工股份有限公司 | Method for producing gasoline rich in aromatic hydrocarbon |
| US11517887B2 (en) | 2018-08-17 | 2022-12-06 | China Petroleum & Chemical Corporation | Modified Y-type molecular sieve, catalytic cracking catalyst comprising the same, their preparation and application thereof |
| SG11202011585VA (en) | 2018-08-17 | 2020-12-30 | China Petroleum & Chem Corp | Modified y-type molecular sieve, catalytic cracking catalyst comprising the same, their preparation and application thereof |
| US11541377B2 (en) | 2018-08-20 | 2023-01-03 | China Petroleum & Chemical Corporation | Modified Y-type molecular sieve, catalytic cracking catalyst comprising the same, their preparation and application thereof |
| TWI812772B (en) | 2018-08-20 | 2023-08-21 | 大陸商中國石油化工科技開發有限公司 | Modified Y-type molecular sieve, catalytic cracking catalyst containing it, and its preparation and use |
| CN111100710B (en) * | 2018-10-25 | 2022-03-11 | 中国石油化工股份有限公司 | Catalytic cracking method and system |
| CN116515524A (en) * | 2022-07-25 | 2023-08-01 | 中国石油化工股份有限公司 | Method for producing light aromatic hydrocarbon by secondary hydrogenation of inferior diesel oil |
| CN115895722A (en) * | 2022-09-27 | 2023-04-04 | 中国石油化工股份有限公司 | System for preparing light aromatic hydrocarbon from heavy oil raw material |
| CN115895726A (en) * | 2022-11-02 | 2023-04-04 | 中国石油化工股份有限公司 | Method for producing light aromatic hydrocarbon from inferior heavy oil in maximized mode |
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