CN103923699B - A kind of catalysis conversion method of producing high-knock rating gasoline - Google Patents
A kind of catalysis conversion method of producing high-knock rating gasoline Download PDFInfo
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Abstract
Produce a catalysis conversion method for high-knock rating gasoline, inferior heavy recycle oil, residual oil carry out hydrotreatment reaction under hydrogen and hydrogenation catalyst existence, and reaction product isolated obtains gas, naphtha, hydrogenated diesel oil and hydrogenated residue; Wherein hydrogenated diesel oil enters catalytic cracking unit, under existing containing the catalytic cracking catalyst of large pore zeolite, carries out cracking reaction, and it is cut and the slurry oil of 250 ~ 450 DEG C that reaction product isolated obtains dry gas, liquefied gas, gasoline, catalysis light diesel fuel, boiling range; Wherein boiling range is that the cut of 250 ~ 450 DEG C is delivered to residual hydrocracking device and recycled. It is farthest saturated to the aromatic ring in inferior heavy recycle oil that the method makes full use of residual hydrogenation condition, thereby make the diesel oil after hydrogenation in catalytic cracking, maximize production high-knock rating gasoline.
Description
Technical field
The present invention relates to a kind of lower boiling hydrocarbon ils catalysis conversion method of producing, more particularly, is onePlant the method for being produced high-knock rating gasoline by inferior heavy recycle oil.
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 is but always relatively poor, and density is large, and arene content is high, Cetane numberLow, even if be also difficult to reach the diesel oil regulation of increasingly stringent by diesel oil hydrogenation modification technology. In addition,China is along with expanding economy, and gasoline car recoverable amount also increases year by year, high-quality gasoline product one direct-furnishShould not ask. Therefore directly catalytic diesel oil inferior is produced into high-knock rating gasoline just seems particularly importantWith urgent.
CN101469274A disclose a kind of by the heavy petrol of the 100-360 in catalytic cracking product DEG C andLight diesel fuel cut through or without hydrogenation after inject catalyst cracker freshening to produce high-octane rating vapourThe method of oil, the shortcoming of the method is that the light fraction in heavy petrol or light diesel fuel is mainly monocycle virtueHydrocarbon, and if mononuclear aromatics hydrogenation, difficulty that hydrogenation is saturated requires greatly, the hydrogen of mentioning in methodIt is saturated that dividing potential drop 1.0-4.0MPa cannot make it, even if it is also easy to be carried out catalytic cracking freshening after saturated againGenerate gas but not gasoline itself. CN101362960A considers that boiling range is 160-260 DEG C heating up in a steamer justIn point, be mainly mononuclear aromatics, therefore directly its catalytic cracking produced to high-knock rating gasoline.
It is 300-6500F(149-343 DEG C by boiling range that US4943366 discloses one), aromatic hydrocarbon contentBe not less than 50%, API degree is not more than 25 light cycle oil at 600-1000psig(4.1-6.9MPa)Under middle pressure condition, the method for high-knock rating gasoline is produced in hydrocracking. CN101987971A is alsoA kind of combination hydrofinishing and hydrocracked, treated poor ignition quality fuel are produced the method for high-knock rating gasoline. ThisThe shortcoming of a little methods is to have hydrogenation in the process due to cracking on the one hand, so the gasoline of producing is pungentAlkane value is still on the low side; Be that hydrocracking is compared with catalytic cracking on the other hand, severity is relatively low,In product, still comprise a large amount of diesel oil distillates.
Summary of the invention
The object of the invention is to provide on the basis of existing technology a kind of urging of high-knock rating gasoline of producingChange method for transformation.
The catalysis conversion method of production aromatic compound provided by the invention comprises:
(1) inferior heavy recycle oil, residual oil and optional distillate are under hydrogen and hydrogenation catalyst existCarry out hydrotreatment reaction, reaction product isolated obtains gas, naphtha, hydrogenated diesel oil and hydrogenation slagOil;
(2) hydrogenated diesel oil of step (1) gained enters catalytic cracking unit, containing large pore zeoliteUnder catalytic cracking catalyst exists, in 470～560 DEG C of reaction temperatures, pressure 0.15 ~ 0.4MPa, reactionThe weight ratio of weight ratio 3～30, water vapour and the raw material of 0.2 ~ 10 second time, catalyst and raw materialUnder 0.05 ~ 0.6 condition, carry out cracking reaction, reaction product isolated obtain dry gas, liquefied gas, gasoline,Catalysis light diesel fuel, boiling range are 250～450 DEG C of preferably cut and slurry oils of 260～400 DEG C;
(3) boiling range step (2) being obtained be 250～450 DEG C preferably the cut of 260 ~ 400 DEG C deliver toResidual hydrocracking device recycles.
Method provided by the invention is specific as follows:
(1) residual hydrocracking device
The feedstock oil of residual hydrocracking device is residual oil, inferior heavy recycle oil and optional distillate.By weight percentage, inferior heavy recycle oil accounts for 3 ~ 50% of residual hydrocracking device feedstock oil.
Described residual oil is decompression residuum and/or reduced crude.
Described inferior heavy recycle oil can be selected from catalytic cracking unit, coking plant, thermal cracking unit,One or more in coal liquification device. The boiling range of inferior heavy recycle oil is 250 ~ 450 DEG C, is preferably260 ~ 400 DEG C. For catalytic cracking unit, the heavy-cycle oil of indication of the present invention is selected from heavy diesel fuel, oneOne or more in middle recycle oil and recycle oil.
Described distillate is to be selected from vacuum gas oil (VGO), coker gas oil, deasphalted oil, solvent refining to take outOne or more in fuel-displaced. These distillates can add in residual oil, also can not add.
Described residual hydrocracking reaction condition is: hydrogen dividing potential drop 5.0～22.0MPa,, reaction temperature330 ~ 450 DEG C, volume space velocity 0.1～3.0 hour-1, hydrogen to oil volume ratio 350 ~ 2000Nm3/m3。
Described residual oil hydrocatalyst active metal component is selected from group vib metal and/or VIIIFamily's base metal, carrier be selected from aluminium oxide, silica, amorphous aluminum silicide appoint～kind or several.The wherein combination of the preferred nickel-tungsten of metal component nickel-tungsten-cobalt, nickel-molybdenum or cobalt-molybdenum.
Residual hydrogenation equipment at least comprises a reactor and a fractionating column. Hydrogenation reactor can beFixed bed reactors can be also moving-burden bed reactor or fluidized bed reactor.
(2) catalytic cracking unit
The hydrogenated diesel oil of step (1) gained enters catalytic cracking unit, preferably enters separately, also canSeparate with other fcc raw material or enter in the lump catalyst cracker, under the existence of catalyst, carrying outCatalytic cracking reaction, separating reaction oil gas and reclaimable catalyst, wherein reclaimable catalyst successively through stripping,Returning reactor after regeneration, reaction oil gas is isolated to and comprises dry gas, liquefied gas, gasoline, catalysisLight diesel fuel, boiling range are 250～450 DEG C of preferably products such as cut and slurry oil of 260～400 DEG C. Described gasolineOctane number is high, is object product; Described catalysis light diesel fuel boiling range is 180 ~ 250 DEG C preferably 200 ~ 260 DEG C;Described boiling range be 250 ~ 450 DEG C preferably the cut of 260 ~ 400 DEG C comprise in FCC heavy diesel oil, a circulationOne or more in oil, recycle oil, can deliver to residual hydrocracking device and recycle.
The boiling range of described hydrogenated diesel oil (or claiming hydrogenation heavy-cycle oil) is 200 ~ 450 DEG C, preferably200 ~ 400 DEG C. The double ring arene content of hydrogenated diesel oil is less than 30 heavy %, is preferably less than 20 heavy %.
The reactor of catalytic cracking unit can be selected from equal diameter riser, etc. linear speed riser, streamOne of in change bed or reducing riser, can be also formed by equal diameter riser and fluid bed compoundReactor. The present invention to reactor without any restriction.
Described device reaction condition is: reaction temperature 470-560 DEG C of preferred 480-550 DEG C, pressure (absolutelyTo pressure) 0.15～0.4MPa, 0.2 ~ 10 second reaction time, the weight ratio of catalyst and raw material is 3 ~ 30,The weight ratio of water vapour and raw material is 0.05 ~ 0.6.
It is solid acid catalyst that the present invention adopts containing the catalytic cracking catalyst of large pore zeolite, active componentCan be selected from containing or not containing the Y of rare earth or HY type zeolite, containing or not containing the ultrastable of rare earth,The carrier of catalyst is artificial synthetic inorganic oxide and natural clay (as kaolin).
The invention has the advantages that:
1, inferior heavy recycle oil being sent into residual hydrogenation equipment, to carry out hydrogenation saturated, can avoid newly-built addingHydrogen production device, thus equipment investment saved;
2, make full use of residual hydrogenation condition farthest saturated to the aromatic ring in inferior heavy recycle oil,Thereby make the diesel oil after hydrogenation in catalytic cracking, maximize production high-knock rating gasoline;
3, in residual oil, add inferior heavy recycle oil, can significantly reduce charging viscosity, thereby can improveThe diffusivity of reactant and removing impurities qualitative response speed, reduce the sulphur, nickel, the content of vanadium that generate in oil,Or increase substantially raw material air speed.
Although Special attention will be given to of the present invention is first sent inferior heavy recycle oil into residual hydrogenation equipment, to carry out hydrogenation fullWith, but not thereby limiting the invention, the independent hydrogenation plant of inferior heavy recycle oil being sent into otherThe hydrogenation that (as Wax Oil Hydrogenation Unit, diesel hydrotreating unit) carries out high severity is saturated, as long as hydrogenationThe double ring arene content of diesel oil is less than 30 heavy %, then by the method for hydrogenated diesel oil again catalytic cracking alsoBelong to the present invention.
Brief description of the drawings
Accompanying drawing is the catalysis conversion method schematic flow sheet of production high-knock rating gasoline provided by the invention.
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 the catalysis conversion method flow process signal of production high-knock rating gasoline provided by the inventionFigure.
Fig. 1 is the schematic flow sheet of preferred forms of the present invention, but does not limit the present invention. IfStandby and the shape of pipeline, the restriction that size is not subject to accompanying drawing, but determine as the case may be. Accompanying drawingIn each numbering be described as follows:
1,2,3,5-8,10-18 all represent pipeline; 4 is residual hydrogenation equipment; 9 is catalytic crackingDevice.
Below in conjunction with accompanying drawing, preferred forms provided by the present invention is further described.
Inferior heavy recycle oil converges through pipeline 18 with from the residual oil of pipeline 2 after pipeline 1,17 mixesAfter enter residual hydrogenation equipment 4, hydrogen enters residual hydrogenation equipment 4 through pipeline 3, at hydrogenation catalystUnder existence, react, separate residual hydrogenation product, obtain gas, hydrotreated naphtha, hydrogenationDiesel oil and hydrogenated residue, wherein gas, hydrotreated naphtha and hydrogenated residue are respectively through pipeline 5,6,8Ejector. Hydrogenated residue need to carry out catalyzed cracking processing, and its catalysis that can enter in accompanying drawing is splitGasifying device 9 is processed, or enters other catalytic cracking unit processing, preferably enters other catalysis and splitsGasifying device processing. Hydrogenated diesel oil enters catalytic cracking unit 9 through pipeline 7, exists in Cracking catalystUnder carry out catalytic cracking reaction, the product of heavy oil separation catalytic cracking, obtain dry gas, liquefied gas,Gasoline, catalysis light diesel fuel, boiling range are 250 ~ 450 DEG C of preferably cut and slurry oils of 260 ~ 400 DEG C, whereinDry gas, liquefied gas, gasoline, catalysis light diesel fuel, slurry oil are respectively through pipeline 10,11,12,13,15Ejector, and boiling range be 250 ~ 450 DEG C preferably 260 ~ 400 DEG C cut successively through pipeline 14,16,17 and converge through pipeline 18 and return to residual hydrogenation equipment from the bad heavy-cycle oil of pipeline 1. Gasoline is pungentAlkane value is high, is object product.
Embodiment
The following examples will be further described the present invention, but not thereby limiting the invention.In embodiment, in hydrotreatment fixed bed reaction district, the catalyst business trade mark of filling is respectivelyRG-10A/RG-10B/RMS-1/RN-32V, admission space ratio is 4:4:15:77, by Chinese stoneChanging catalyst branch company produces. The catalyst board of filling in hydro-upgrading fixed bed reaction district in comparative exampleNumber be respectively FH-98/3963, admission space ratio is 40/60.
The catalyst business trade mark that catalytic cracking unit uses is MLC-500, by Sinopec catalystBranch company produces, and fresh catalyst is through 800 DEG C, 100% steam aging 17 hours, character and oldActivity after change is in table 1.
The feedstock oil character using in embodiment, comparative example is listed in table 2.
Embodiment 1
The present embodiment explanation adopts method provided by the invention, raw material through kitty cracker and inThe situation of the product distribution after treatment of type residual hydrocracking device and product property.
The feedstock oil that enters residual hydrogenation equipment is the mixed of decompression residuum, catalytic cracking inferior heavy recycle oilCompound, the mass ratio of the two is 90:10. The experimental condition of residual hydrogenation is: hydrogen dividing potential drop 14.2MPa,400 DEG C of reaction temperatures, hydrogen-oil ratio 1000Nm3/m3, air speed is 0.28h-1。
Hydrogenation products diesel oil (boiling range 200-380 DEG C) is as catalytically cracked material, the test of catalytic crackingCondition is: 510 DEG C of reaction temperatures, and oil ratio is 6:1, and water-oil factor is 0.1, and the reaction time is 3.2Second.
Comparative example 1
Medium-sized tester is identical with embodiment 1 with catalyst. Just catalytic cracking inferior heavy is followedRing oil carries out hydrotreatment separately, the test of diesel oil hydrogenation modification on medium-sized diesel oil hydrogenation modification deviceCondition is: hydrogen dividing potential drop 5.2MPa, 350 DEG C of reaction temperatures, hydrogen-oil ratio 400Nm3/m3, air speed is 1.5h-1。
Hydrogenation products diesel oil (boiling range 200-380 DEG C) is as catalytically cracked material, the test of catalytic crackingCondition is: 510 DEG C of reaction temperatures, and oil ratio is 6:1, and water-oil factor is 0.1, and the reaction time is 3.2Second.
Comparative example 2
Medium-sized tester is identical with embodiment 1 with catalyst. Just catalytic cracking inferior heavy is followedRing oil is without the saturated processing of any hydrogenation, directly as catalytically cracked material. The test bar of catalytic crackingPart is: 510 DEG C of reaction temperatures, and oil ratio is 6:1, and water-oil factor is 0.1, and the reaction time is 3.2 seconds.
Device operating condition is in table 3, and the diesel oil mass spectrum after hydrogenation forms in table 4, and catalytic cracking product dividesCloth is in table 5.
Comparative example and comparative example can find, although hydrogen dividing potential drop, reaction temperature, hydrogen in embodimentIt is high that oil ratio geometric ratio comparative example is wanted, but can find in the diesel oil after hydrogenation, only to contain seldom in embodimentAromatic hydrocarbons, and be mainly mononuclear aromatics, other is mainly cycloalkane, finally causes the catalysis of embodimentDuring crackate distributes, gasoline yield, up to 60 heavy %, exceeds approximately 13 percentage points of comparative examples 1, heightGo out approximately 18 percentage points of comparative examples 2; In embodiment, total liquid is received up to 93 heavy %, correspondingly exceeds contrastApproximately 4 percentage points of examples 1, exceed approximately 8 percentage points of comparative examples 2. Gasoline in embodiment is pungent simultaneouslyAlkane value RON is up to more than 100.
Table 1
| Catalyst | |
| Chemical composition, heavy % | |
| Aluminium oxide | 49.5 |
| Sodium oxide molybdena | 0.05 |
| Apparent density, kg/m3 | 865 |
| Pore volume, ml/g | 0.2 |
| Specific area, rice2/ gram | 145 |
| Abrasion index, heavy % hour-1 | 1.6 |
| Size consist, heavy % | |
| 0～40 micron | 15.8 |
| 40～80 microns | 65.9 |
| > 80 microns | 18.3 |
| Active (800 DEG C, 17h-1），% | 62 |
Table 2
| Feedstock oil title | Inferior heavy recycle oil |
| Existent gum, mg/100mL | 975.2 |
| Freezing point, DEG C | -14 |
| Aniline point, DEG C | <25 |
| 10% carbon residue, heavy % | 0.69 |
| Mean molecule quantity | 177 |
| Boiling range, DEG C | |
| Initial boiling point | 246 |
| 5% | 260 |
| 10% | 264 |
| 30% | 282 |
| 50% | 303 |
| 70% | 328 |
| 90% | 357 |
| 95% | 368 |
| The end point of distillation | 370 |
| Mass spectrography quality composition, % | |
| Alkane | 10.3 |
| Total cycloalkane | 4.8 |
| Total aromatic hydrocarbons | 83.9 |
| Mononuclear aromatics | 12.2 |
| Double ring arene | 59.9 |
| Gross mass | 100.0 |
Table 3
| Embodiment 1 | Comparative example 1 | Comparative example 2 | |
| Operating condition | |||
| Catalytic unit | |||
| Reaction temperature, DEG C | 510 | 510 | 510 |
| The time of staying, second | 3.2 | 3.2 | 3.2 |
| Oil ratio | 6.0 | 6.0 | 6.0 |
| Water-oil factor | 0.1 | 0.1 | 0.1 |
| Hydrogenation unit | |||
| Hydrogen dividing potential drop, MPa | 14.2 | 5.2 | _ |
| Reaction temperature, DEG C | 400 | 350 | - |
| Cumulative volume air speed, h-1 | 0.28 | 1.5 | - |
| Hydrogen to oil volume ratio, Nm3/m3 | 1000 | 400 | - |
Table 4
| Embodiment 1 | Comparative example 1 | Comparative example 2 | |
| Mass spectrography quality composition, % | |||
| Alkane | 2.6 | 4.2 | 10.3 |
| Total cycloalkane | 86.8 | 55.0 | 4.8 |
| Total aromatic hydrocarbons | 10.6 | 40.8 | 83.9 |
| Mononuclear aromatics | 10.6 | 35.2 | 12.2 |
| Double ring arene | 0.0 | 5.6 | 59.9 |
| Gross mass | 100.0 | 100.0 | 100.0 |
Table 5
| Embodiment 1 | Comparative example 1 | Comparative example 2 | |
| Product distributes, heavy % | |||
| Dry gas | 1.90 | 1.60 | 1.60 |
| Liquefied gas | 15.60 | 13.86 | 12.78 |
| Gasoline | 59.94 | 46.14 | 31.72 |
| Light diesel fuel | 17.55 | 29.30 | 40.50 |
| Heavy oil | 1.00 | 3.40 | 5.58 |
| Coke | 4.01 | 5.70 | 7.82 |
| Add up to | 100.00 | 100.00 | 100.00 |
| Total liquid yield, heavy % | 93.09 | 89.3 | 85.0 |
| Octane number | |||
| RON | 101.6 | 98.5 | 98.9 |
| MON | 90.5 | 87.6 | 87.8 |
Claims (13)
1. produce a catalysis conversion method for high-knock rating gasoline, it is characterized in that the method comprises:
(1) inferior heavy recycle oil, residual oil and optional distillate are under hydrogen and hydrogenation catalyst existCarry out hydrotreatment reaction, reaction product isolated obtains gas, naphtha, hydrogenated diesel oil and hydrogenation slagOil;
(2) hydrogenated diesel oil of step (1) gained enters catalytic cracking unit, containing large pore zeoliteCatalytic cracking catalyst carries out cracking reaction under existing, at 470～560 DEG C of reaction temperatures, pressureWeight ratio 3～30, the water vapour of 0.15～0.4MPa, 0.2～10 second reaction time, catalyst and raw materialWith under the condition of the weight ratio 0.05～0.6 of raw material, carry out cracking reaction, reaction product isolated obtain dry gas,Liquefied gas, gasoline, catalysis light diesel fuel, boiling range are cut and the slurry oil of 250～450 DEG C, described hydrogenationThe boiling range of diesel oil is 200～450 DEG C, and the double ring arene content of hydrogenated diesel oil is less than 30 heavy %;
(3) boiling range step (2) being obtained is that the cut of 250～450 DEG C is delivered to residual hydrocrackingDevice recycles.
2. according to the method for claim 1, it is characterized in that the boiling range of described inferior heavy recycle oil is250～450℃。
3. according to the method for claim 2, it is characterized in that the boiling range of described inferior heavy recycle oil is260～400℃。
4. according to the method for claim 1, it is characterized in that described inferior heavy recycle oil carrys out catalytic crackingOne or more in device, coking plant, thermal cracking unit, coal liquification device.
5. according to the method for claim 4, it is characterized in that described inferior heavy recycle oil carrys out catalytic crackingOne or more in device heavy diesel fuel, one in recycle oil and recycle oil.
6. according to the method for claim 1, it is characterized in that described distillate be selected from vacuum gas oil (VGO),One or more in oil are extracted in coker gas oil, deasphalted oil, solvent refining out.
7. according to the method for claim 1, it is characterized in that hydrotreatment reaction condition is: hydrogen dividing potential drop5.0～22.0MPa, 330～450 DEG C of reaction temperatures, volume space velocity 0.1～3.0 hour-1, hydrogen to oil volume ratio350～2000Nm3/m3。
8. according to the method for claim 1, it is characterized in that the sorting of described activity of hydrocatalyst metal groupFrom group vib metal and/or group VIII base metal, carrier be selected from aluminium oxide, silica,Any one or several in amorphous aluminum silicide.
9. according to the method for claim 8, it is characterized in that described metal component be selected from nickel-tungsten, nickel-tungsten-The combination of cobalt, nickel-molybdenum or cobalt-molybdenum.
10. according to the method for claim 1, it is characterized in that the boiling range of described hydrogenated diesel oil is200～400 DEG C. The double ring arene content of hydrogenated diesel oil is less than 20 heavy %.
11. according to the method for claim 1, it is characterized in that the described reaction temperature of step (2) is480～550℃。
12. according to the method for claim 1, it is characterized in that described 250～450 DEG C of step (2), (3)Cut comprise one or more in recycle oil, recycle oil in FCC heavy diesel oil.
13. according to the method for claim 1, and the catalytic cracking containing large pore zeolite described in it is characterized in that is urgedAgent active component can be selected from containing or not containing the Y of rare earth or HY type zeolite, containing or containing rare earthUltrastable.
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| US9777229B2 (en) * | 2015-03-10 | 2017-10-03 | Uop Llc | Process and apparatus for hydroprocessing and cracking hydrocarbons |
| CN109679687B (en) * | 2017-10-19 | 2021-06-11 | 中国石油化工股份有限公司 | Catalytic conversion method for producing low-benzene high-octane gasoline |
| CN111100709A (en) * | 2018-10-25 | 2020-05-05 | 中国石油化工股份有限公司 | Method for producing high-value chemical products by adopting inferior LCO |
| CN111647430B (en) * | 2019-03-04 | 2022-01-04 | 中国石油化工股份有限公司 | Treatment method and system for inferior oil |
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| CN102816594A (en) * | 2011-06-10 | 2012-12-12 | 中国石油天然气股份有限公司 | Residual oil hydrotreating-catalytic cracking-solvent refining combined process |
| CN102816597A (en) * | 2011-06-10 | 2012-12-12 | 中国石油天然气股份有限公司 | Residual oil hydrotreating process |
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| CN102816594A (en) * | 2011-06-10 | 2012-12-12 | 中国石油天然气股份有限公司 | Residual oil hydrotreating-catalytic cracking-solvent refining combined process |
| CN102816597A (en) * | 2011-06-10 | 2012-12-12 | 中国石油天然气股份有限公司 | Residual oil hydrotreating process |
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