CN104560166A - Catalytic conversion method utilizing petroleum hydrocarbon to produce high-octane gasoline - Google Patents
Catalytic conversion method utilizing petroleum hydrocarbon to produce high-octane gasoline 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
A catalytic conversion method utilizing petroleum hydrocarbon to produce high-octane gasoline comprises the following steps: light catalytic cycle oil is cut to obtain light fractions and heavy fractions, the heavy fractions are subjected to hydrotreatment to obtain hydrogenized heavy fractions, the light fractions and the hydrogenized heavy fractions separately enter an auxiliary riser reactor of a catalytic cracking unit, heavy petroleum hydrocarbons enter a main riser reactor of the catalytic cracking unit, cracking reaction is realized in the presence of a catalytic cracking catalyst, and the resultant is separated to obtain products including gasolene and light cycle oil. According to the invention, the light fractions of light cycle oil and the hydrogenized heavy fractions enter the auxiliary riser reactor layer by layer, so that severe conditions required for catalytic cracking reaction of different fractions of light cycle oil can be optimized and satisfied to the utmost extent, and accordingly, high-octane catalytic gasoline can be produced to the maximum extent.
Description
Technical field
The invention belongs to the catalysis conversion method of petroleum hydrocarbon in the absence of hydrogen, more particularly, is a kind of catalysis conversion method being produced stop bracket gasoline by heavy petroleum hydrocarbon.
Background technology
Along with the development of crude oil heaviness and market are to the quick growth of light-end products demand, in China, the catalytic cracking technology as heavy oil lighting is rapidly developed.But, must faced by a fact be that the quality of catalytic cracking diesel oil (or claim " light cycle oil ") is but always relatively poor, density is large, and aromaticity content is high, cetane value is low, even if be also difficult to by diesel oil hydrogenation modification technology the diesel oil regulation reaching increasingly stringent.How solving catalytic cracking light cycle oil is an increasingly serious problem.Simultaneous another one problem is domestic gasoline product chronic shortage, and catalytically cracked gasoline accounts for 80% of gasoline product.Therefore, how to realize heavy feed stock maximization production stop bracket gasoline and not produce light cycle oil may being the new way solved the problem by catalytic cracking process.
US4585545 discloses one and complete for catalytic cracking light cycle oil cut is first carried out hydrotreatment, and the hydrogenated diesel oil obtained goes catalytic cracking to produce the catalysis conversion method being rich in mononuclear aromatics gasoline again.
CN1422327A discloses a kind of method of catalytic cracking light cycle oil upgrading, is the light cycle oil that the first catalytic cracking unit taking mink cell focus as raw material is produced is carried out deep hydrogenation, and the hydrogenation turning oil obtained enters the second catalytic cracking unit again.On the basis of the method, CN1423689A emphasizes that catalyst requirement in the second catalytic cracking unit is more than or equal to the large pore zeolite of about 0.7nm, optionally to improve light olefins yields containing the aperture of selecting shape zeolite and about 5-50% of 50-95%.
CN1466619A discloses a kind of method for transformation of catalytic cracking light cycle oil, that catalytic cracking riser reactor is divided into upstream and downstream two reaction zones, wherein mink cell focus injects catchment, and the hydrogenation turning oil that its catalytic cracking production light cycle oil obtains after hydrotreatment injects upstream.On the basis of the method, the charging in CN1425054A method middle and lower reaches district, except hydrogenation turning oil, also add petroleum naphtha.In the method, not only hydrogen consumption is high, and hydrogenation turning oil can have a strong impact on the conversion of the mink cell focus in downstream in upstream reaction.
Can find from disclosed document above, catalytic cracking light cycle oil being carried out to one of important channel processed is that it is first carried out hydrotreatment, and then catalytic cracking.It must be noted that, light cycle oil no matter whether hydrogenation, compare, its molecule is little with mink cell focus macromole, bond energy is large, the operating parameters therefore how controlling catalytic cracking is one of key of light cycle oil processing.If light cycle oil carries out hydrogenation simultaneously, the operation control of hydrogenation process is also one of key of light cycle oil processing.In addition, maximize in heavy petroleum hydrocarbon catalytic cracking process and produce stop bracket gasoline and do not produce light cycle oil, then must take into account the selective catalysis cracking how consideration realizes heavy petroleum hydrocarbon and light cycle oil.
Summary of the invention
The object of the invention is to provide a kind of on the basis of existing technology and maximized the catalysis conversion method producing stop bracket gasoline by heavy petroleum hydrocarbon.
Catalysis conversion method provided by the invention comprises:
(1) catalytic cracking light cycle oil obtains lighting end and last running through cutting;
(2) step (1) described last running carries out hydrotreatment reaction under hydrogen and hydrotreating catalyst exist, and reaction product isolated obtains hydrogenation last running;
(3) step (1) described lighting end, the described hydrogenation last running of step (2) layering from bottom to up enter the secondary riser reactor of catalytic cracking unit, catalytic cracking reaction is carried out under catalytic cracking catalyst exists, be separated catalytic cracking catalyst to be generated and reaction oil gas, wherein reaction oil gas is isolated to the product comprising gasoline, light cycle oil;
(4) heavy crude hydrocarbon feed enters the main riser reactor of catalytic cracking unit, catalytic cracking reaction is carried out under catalytic cracking catalyst exists, be separated catalytic cracking catalyst to be generated and reaction oil gas, wherein reaction oil gas is isolated to the product comprising gasoline, light cycle oil;
(5) step (3), (4) described catalytic cracking catalyst to be generated gained regeneration catalyzing cracking catalyst after stripping, regeneration returns riser reactor and recycles.
The described catalytic cracking light cycle oil of step (1) be selected from allocatalysis cracking unit produce light cycle oil or/and present method catalytic cracking unit step (3) produce light cycle oil, preferred allocatalysis light cycle oil that cracking unit produces and present method catalytic cracking unit step (3) produce light cycle oil.In aforesaid method, step (3) is called light cycle oil recycle ratio with the mass ratio of heavy crude hydrocarbon feed.
Method provided by the invention is specific as follows:
Catalytic cracking light cycle oil enters independent separation column and cuts, cutting temperature controls at 250 ~ 260 DEG C, preferred cutting temperature is 260 DEG C, obtains respectively not higher than the lighting end of this cutting temperature and the last running higher than this cutting temperature from the top of separation column and bottom.
Hydrotreater is removed in described last running, and under hydrogen and hydrogenation catalyst exist, carry out hydrotreatment reaction, hydroprocessing condition is: hydrogen dividing potential drop 5.0 ~ 22.0MPa, preferably 8.0 ~ 15.0MPa; Temperature of reaction 330 ~ 450 DEG C, preferably 340 ~ 380 DEG C; Volume space velocity 0.1 ~ 10.0 hour
-1, hydrogen to oil volume ratio 100 ~ 2000Nm
3/ m
3.Reaction product isolated obtains the cut of the preferred > of initial boiling point > 250 DEG C 260 DEG C, or claims hydrogenated diesel oil, hydrogenation last running.In described hydrogenation last running, two ring aromatic content wants≤20 heavy %, the heavy % in preferably≤10.
Described activity of hydrocatalyst metal component is selected from group vib metal and/or group VIII base metal, in support selected from alumina, silicon-dioxide, amorphous aluminum silicide any one or several.Described group vib metal be molybdenum or/and tungsten, group VIII base metal is that nickel is or/and cobalt.The combination of the preferred nickel-tungsten of active metal component, nickel-tungsten-cobalt, nickel-molybdenum or cobalt-molybdenum.
A part of high-temperature regenerated catalyst from revivifier enters the pre lift zone bottom riser reactor, promotes, up through pre-lift medium, with lighting end contact reacts, up; Subsequently with hydrogenation last running contact reacts, oil gas, catalyst mixture are up, then with heavy crude hydrocarbon feed, another part high-temperature regenerated catalyst contact reacts from revivifier; Reaction oil gas from riser tube out after finally enter main fractionating tower and absorbing-stabilizing system subsequently and then separation.Wherein main fractionating tower light cycle oil out can enter newly-increased light cycle oil separation column and cuts, cut the light cycle oil lighting end direct circulation obtained and return secondary riser tube, and the light cycle oil last running that cutting obtains goes hydrotreater to carry out hydrotreated lube base oil, and the light cycle oil last running after hydrogenation loops back secondary riser tube.
The lighting end of light cycle oil and hydrogenation last running preferably separately enter separately the secondary riser reactor of catalytic cracking unit, and wherein lighting end enters from the underlying nozzle (upstream) of riser tube, and hydrogenation last running enters from the upper strata nozzle (downstream) of riser tube.The distance of upper and lower layer nozzle is be advisable for 0.01 ~ 3 second to control the residence time of reaction oil gas in two-layer nozzle distance, preferably 0.05 ~ 1 second.The advantage that lighting end and hydrogenation last running layering enter to optimize the reaction conditions meeting different fractions catalytic cracking, thus realize farthest transforming.
The reaction conditions of the main riser reactor of catalytic cracking unit is not particularly limited, as conventional heavy oil fluid catalytic cracking condition, temperature of reaction is 450-550 DEG C, agent oil quality is than 4 ~ 8,2 ~ 4 seconds oil gas residence time, pressure (absolute pressure) 0.15 ~ 0.4MPa, the weight ratio of water vapor and raw material is 0.02 ~ 0.08; The raw material of main riser reactor and heavy petroleum hydrocarbon are also not particularly limited, conventional heavy feed stock.The described heavy crude hydrocarbon feed of step (3) is selected from one or more in straight-run gas oil, wax tailings, deasphalted oil, hydrofined oil, hydrocracking tail oil, vacuum residuum, long residuum.
The reaction conditions of secondary riser reactor is: temperature of reaction is 520 ~ 650 DEG C, preferably 550 ~ 590 DEG C; Agent oil quality than 5 ~ 100, preferably 8 ~ 50; 1 ~ 10 second oil gas residence time, preferably 2 ~ 8 seconds; Pressure (absolute pressure) 0.15 ~ 0.4MPa; The weight ratio of water vapor and raw material is 0.01 ~ 0.5 preferably 0.02 ~ 0.2.
The equilibrium catalyst agent activity (MAT) >=60 of catalytic cracking unit, preferably >=62.
The described secondary riser reactor of step (3), the described main riser reactor of step (4), be isometrical riser reactor or reducing riser reactor.Secondary riser reactor and main riser reactor can share a set of settling vessel, main fractionating tower, absorbing-stabilizing system, stripper, revivifier, also can use respective settling vessel, main fractionating tower, absorbing-stabilizing system, stripper, revivifier.
Catalytic cracking catalyst comprises zeolite, inorganic oxide and optional clay.The content of each component is respectively: the heavy % of the heavy % of zeolite 10 ~ 50, the heavy % of inorganic oxide 5 ~ 90, clay 0 ~ 70.Wherein active ingredient be selected from containing or not containing rare earth Y, HY, USY or Beta zeolite in one, two or more.
The invention has the advantages that:
1, thoroughly can realize heavy crude hydrocarbon catalytic cracking and not produce light cycle oil.
2, catalytic cracking unit light cycle oil is first cut, and wherein last running will remove hydrogenation, hydrogen consumption can be reduced to greatest extent;
3, adopt the major and minor riser tube of catalytic cracking unit to process heavy petroleum hydrocarbon and light cycle oil respectively, contribute to the operational condition optimizing the two respectively, the maximization of both realizations transforms.
4, the last running layering in secondary riser reactor after the lighting end of light cycle oil and hydrogenation enters, the severe condition met needed for light cycle oil different fractions catalytic cracking reaction can be optimized to greatest extent, thus farthest produce high-octane catalytic gasoline.
Accompanying drawing explanation
Fig. 1 is the catalysis conversion method schematic flow sheet of production high-octane rating catalytic gasoline provided by the invention.
Embodiment
Further illustrate method provided by the present invention below in conjunction with accompanying drawing, but the present invention is not therefore 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.Shape, the size of equipment and pipeline not by the restriction of accompanying drawing, but are determined as the case may be.In accompanying drawing, each numbering is described as follows:
1,3-5,7,13,15-16,18-20,22 all represent pipeline; 2 is light cycle oil separation column; 6 is hydrotreater; 10 is catalytic cracking unit; 8,9,21 is feed nozzle; 11 is secondary riser reactor; 12 is main riser reactor; 14 is main fractionating tower; 17 is absorbing-stabilizing system.
Below in conjunction with accompanying drawing, preferred forms provided by the present invention is further described.
The main riser reactor 12 that heavy crude hydrocarbon feed enters catalytic cracking unit 10 through nozzle 21 carries out catalytic cracking reaction, and reaction oil gas enters main fractionating tower 14 through pipeline 13, from main fractionating tower 14 slurry oil out through pipeline 15 as product discharger; Enter follow-up absorbing-stabilizing system 17 from main fractionating tower 14 oil gas out through pipeline 16 to be separated further and to obtain product dry gas, liquefied gas and stop bracket gasoline, respectively from pipeline 18,19,20 caterpillar; And main fractionating tower 14 light cycle oil out enters light cycle oil separation column 2 through pipeline 22,1 cuts, obtain≤lighting end of 260 DEG C and the last running of > 260 DEG C.The lighting end of wherein≤260 DEG C enters the underlying nozzle 9 of the secondary riser reactor 11 of catalytic cracking reaction device 10 through pipeline 3; And the last running of > 260 DEG C enters hydrotreater 6 through pipeline 4, hydrogen introduces hydrotreater 6 through pipeline 5 simultaneously.Product hydrogenation last running after hydrogenation also enters the upper strata nozzle 8 of the secondary riser reactor 11 of catalytic cracking reaction device 10 through pipeline 7.There is catalytic cracking reaction in lighting end and hydrogenation last running, reaction oil gas also enters main fractionating tower 14 through pipeline 13 and goes to carry out later separation in secondary riser reactor under cracking catalyst exists.
The following examples will be further described the present invention, but not thereby limiting the invention.In embodiment, in hydrotreatment fixed-bed reactor, the hydrotreating catalyst commercial grades of filling is RN-32V; protective material commercial grades is RG-1; hydrotreating catalyst and protectant admission space ratio are 95:5, produce by Sinopec catalyzer branch office.
In embodiment, comparative example, the physico-chemical property of the catalyzer that catalytic cracking unit uses is in table 1, and its commercial grades is HAC, is produced by Sinopec catalyzer branch office.
The heavy crude hydrocarbon feed used in embodiment, comparative example is the mixing raw material of 90 heavy % straight-run gas oils and 10 heavy % vacuum residuum, and its character lists in table 2.
Embodiment
The present embodiment illustrates the method adopting and provide in Fig. 1 of the present invention.Wherein the boiling range cutting temperature of light cycle oil separation column is 250 DEG C.
Light cycle oil last running enters medium-sized hydrotreater, and the test conditions of hydrotreatment is: hydrogen dividing potential drop 8.0MPa; Average bed temperature of reaction 360 DEG C, volume space velocity 0.5 hour
-1, hydrogen to oil volume ratio 1100Nm
3/ m
3.In hydrogenation last running, two ring aromatic content is 8.0 heavy %.
The main operating parameters of catalytic cracking unit is in table 3.Lighting end enters from the underlying nozzle of secondary riser tube, and hydrogenation last running enters from the upper strata nozzle of secondary riser tube, and the residence time of distance controlling reaction oil gas in two-layer nozzle distance of upper and lower layer nozzle is 0.2 second.
Comparative example
In comparative example, catalytic cracking test device only has main riser tube, does not have secondary riser tube.Light cycle oil separation column is not had in comparative example yet.The light cycle oil that in comparative example, main fractionating tower obtains directly goes hydrogenation unit to carry out hydrogenation of total effluent without cutting, enters the main riser reactor reaction of catalytic cracking unit after the light cycle oil after hydrogenation and heavy crude hydrocarbon feed are mixed together.In comparative example, catalyzer is identical with embodiment.The operational condition of the catalytic cracking unit of comparative example is in table 3.
Catalytic cracking product distribution, hydrogen consumption and gasoline octane rating are in table 4.
Comparative example and comparative example can find, embodiment obviously can reduce hydrogen consumption in hydrogenation process, and hydrogen consumption is reduced to 1.43% from 2.6%; In addition, because the recycle ratio of light cycle oil is 0.29 in comparative example, far above 0.07 in embodiment, finally cause its energy consumption higher.Can also find, compare ratio, in embodiment, gasoline yield increases percentage point more than 9 simultaneously, and dry gas and coke yield obviously reduce simultaneously.In addition, as can be found from Table 4, compare ratio, the product gasoline octane value RON in embodiment is increased to 95.8 by 92.1.
Table 1 HAC catalyst property
Table 2 stock oil character
| Stock oil title | Mixing raw material |
| Density (20 DEG C), kg/m 3 | 916.8 |
| Zero pour, DEG C | 32 |
| Specific refractory power (70 DEG C) | 1.4968 |
| Carbon residue, heavy % | 2.67 |
| Molecular-weight average | 404 |
| Boiling range, DEG C | |
| Initial boiling point | 294 |
| 5% | 361 |
| 10% | 381 |
| 30% | 422 |
| 50% | 451 |
| 70% | 497 |
| Sulphur content, % | 1.1 |
| Nitrogen content, % | 0.24 |
| Hydrogen richness, % | 12.6 |
| Metal content, mg/kg | |
| Ni | 6.6 |
| V | 1.2 |
Table 3 operating parameters
Table 4
| Embodiment | Comparative example | |
| Hydrogen consumes, % | 1.43 | 2.6 |
| Energy consumption, kg marks oil/ton raw material | 69 | 76 |
| Product slates, heavy % | ||
| Dry gas | 3.21 | 5.57 |
| Liquefied gas | 17.61 | 22.58 |
| Gasoline | 65.63 | 56.47 |
| Solar oil | 0.00 | 0.00 |
| Heavy oil | 4.51 | 3.11 |
| Coke | 9.04 | 12.27 |
| Add up to | 100.00 | 100.00 |
| Gasoline octane rating | ||
| RON | 95.8 | 92.1 |
| MON | 85.2 | 81.6 |
Claims (15)
1. petroleum hydrocarbon produces a catalysis conversion method for stop bracket gasoline, it is characterized in that the method comprises:
(1) catalytic cracking light cycle oil obtains lighting end and last running through cutting;
(2) step (1) described last running carries out hydrotreatment reaction under hydrogen and hydrotreating catalyst exist, and reaction product isolated obtains hydrogenation last running;
(3) step (1) described lighting end, the described hydrogenation last running of step (2) layering from bottom to up enter the secondary riser reactor of catalytic cracking unit, catalytic cracking reaction is carried out under catalytic cracking catalyst exists, be separated catalytic cracking catalyst to be generated and reaction oil gas, wherein reaction oil gas is isolated to the product comprising gasoline, light cycle oil;
(4) heavy crude hydrocarbon feed enters the main riser reactor of catalytic cracking unit, catalytic cracking reaction is carried out under catalytic cracking catalyst exists, be separated catalytic cracking catalyst to be generated and reaction oil gas, wherein reaction oil gas is isolated to the product comprising gasoline, light cycle oil;
(5) step (3), (4) described catalytic cracking catalyst to be generated gained regeneration catalyzing cracking catalyst after stripping, regeneration returns riser reactor and recycles.
2., according to the method for claim 1, it is characterized in that step (3) described light cycle oil returns step (1).
3., according to the method for claim 1, it is characterized in that the cutting temperature of described light cycle oil is 250 ~ 260 DEG C.
4., according to the method for claim 1, it is characterized in that the condition of described step (2) described hydrotreatment is hydrogen dividing potential drop 5.0 ~ 22.0MPa, temperature of reaction 330 ~ 450 DEG C, volume space velocity 0.1 ~ 10.0 hour
-1, hydrogen to oil volume ratio 100 ~ 2000Nm
3/ m
3.
5. according to the method for claim 1, it is characterized in that the active metal component of described step (2) described hydrotreating catalyst is selected from group vib metal and/or group VIII base metal, in support selected from alumina, silicon-dioxide, amorphous aluminum silicide any one or several.
6. according to the method for claim 5, 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.
7., according to the method for claim 5, it is characterized in that described active metal component is selected from the combination of nickel-tungsten, nickel-tungsten-cobalt, nickel-molybdenum or cobalt-molybdenum.
8., according to the method for claim 1, it is characterized in that in hydrogenation last running, two ring aromatic content is not more than 20 heavy %.
9., according to the method for claim 1, it is characterized in that the described secondary riser reactor of step (3), the described main riser reactor of step (4) is isometrical riser reactor or reducing riser reactor.
10. according to the method in claim 1, it is characterized in that lighting end and hydrogenation last running separately enter separately the secondary riser reactor of catalytic cracking unit, wherein lighting end enters from the underlying nozzle of secondary riser tube, and hydrogenation last running enters from the upper strata nozzle of secondary riser tube.
11. according to the method in claim 10, it is characterized in that the distance of upper and lower layer nozzle is 0.01 ~ 3 second to control the residence time of reaction oil gas in two-layer nozzle distance.
12. according to the method in claim 1, it is characterized in that the reaction conditions of secondary riser reactor is: temperature of reaction is 520 ~ 650 DEG C, agent oil quality is than 5 ~ 100,1 ~ 10 second oil gas residence time, pressure 0.15 ~ 0.4MPa, the weight ratio of water vapor and raw material is 0.01 ~ 0.5, and the activity of device equilibrium catalyst is not less than 60.
13. according to the method in claim 12, it is characterized in that the reaction conditions of secondary riser reactor is: temperature of reaction is 550 ~ 590 DEG C, agent oil quality is than 8 ~ 50,2 ~ 8 seconds oil gas residence time, the weight ratio of water vapor and raw material is 0.02 ~ 0.2, and the activity of device equilibrium catalyst is not less than 62.
14. according to the method for claim 1, it is characterized in that step (3) described catalytic cracking catalyst comprises zeolite, inorganic oxide and optional clay, the content of each component is respectively: the heavy % of the heavy % of zeolite 10 ~ 50, the heavy % of inorganic oxide 5 ~ 90, clay 0 ~ 70, wherein active ingredient be selected from containing or not containing Y, HY, USY or Beta zeolite of rare earth one, two or more.
15. according to the method for claim 1, it is characterized in that the described heavy crude hydrocarbon feed of step (3) is selected from straight-run gas oil, wax tailings, deasphalted oil, hydrofined oil, hydrocracking tail oil, vacuum residuum, long residuum one or more.
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| US10808188B2 (en) | 2017-09-26 | 2020-10-20 | China Petroleum & Chemical Corporation | Catalytic cracking process with increased production of a gasoline having a low olefin content and a high octane number |
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| CN104560166B (en) | 2016-05-25 |
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