CN103805247A - Combination method used for processing inferior diesel oil - Google Patents
Combination method used for processing inferior diesel oil Download PDFInfo
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Abstract
The invention discloses a combination method used for processing inferior diesel oil. According to the combination method used for processing inferior diesel oil, secondary processing of inferior diesel fractions comprises following steps: hydro-upgrading reaction is carried out firstly, and aromatic hydrocarbon selective ring-opening reaction is carried out; a reaction effluent is separated so as to obtain a liquid material, and the liquid material is extracted; aromatic hydrocarbon components are taken as catalytic cracking raw materials and are subjected to catalytic cracking reaction, and a gas material, catalytic gasoline and catalytic diesel oil are obtained via separation and fractionation; and catalytic diesel oil can be recycled back to a hydro-upgrading reactor. The combination method is capable of converting inferior diesel oil into catalytic gasoline products with high octane value as much as possible, increasing gasoline yield and octane value of a catalytic unit as far as possible, and providing an economical feasible technical route for inferior diesel oil processing.
Description
Technical field
The present invention relates to a kind of poor ignition quality fuel treatment process, specifically a kind of combined technical method that is suitable for processing poor quality catalytic cracking diesel raw material.
Background technology
Catalytic cracking is most important secondary processing process in current petroleum refining industry, is also the core process of heavy oil lighting.Along with Global Oil heaviness day by day, the processing power of FCC apparatus also improves constantly, take various mink cell focuses as raw material, obtain main products stop bracket gasoline by catalytic cracking reaction, a large amount of sulphur, nitrogen, aromaticity content have been produced high simultaneously, cetane value or cetane index are low, and the catalytic diesel oil of stability extreme difference.And the requirement of environmental regulation is also day by day harsh, diesel oil index, also progressively improving, all has strict requirement to the sulphur content in product, aromaticity content, cetane index etc. simultaneously.So in reducing the output of this part poor ignition quality fuel, also need to find a kind of suitable method to carry out to it requirement that processing treatment appears on the scene to meet enterprise product.
Hydrocracking technology has the plurality of advantages such as adaptability to raw material is strong, products scheme is flexible, liquid product yield is high, good product quality, is subject to for many years the favor of countries in the world oil refining enterprise always.As the hydrocracking of one of the main technique of heavy oil deep processing not only can direct production vapour, the clean automotive fuel such as coal, bavin, and light, heavy naphtha and hydrocracking tail oil or the industrial chemicals of high-quality in its product, therefore, hydrocracking technology progressively develops into the bridge technology that the modern times refine oil and petroleum chemical enterprise's oil, change, fibre organically combine in recent years.
And in hydrocracking technology, MCI(improves cetane value to greatest extent) technique is as a kind of special means targetedly, can process the poor ignition quality fuel that catalytic cracking produces.Make it make hydro carbons open loop and not chain rupture, can increase substantially the cetane value of catalytic diesel oil and obtain higher diesel yield.The catalyzer that MCI technique is used has hydrogenating desulfurization (HDS), hydrodenitrification (HDN) and hydrogenation saturated activity is high, hydroisomerizing is active high and cracking activity is low and the feature that has good stability, generally the cetane value of catalytic diesel oil can be improved to 10 more than unit.
CN101463274A has introduced a kind of improved hydrocarbon oil hydrogenation and has processed and catalytic cracking combined technique, comprise, first various inferior raw materials are carried out to hydrotreatment, after cutting, goes again the tail oil obtaining to carry out catalytic cracking, can obtain more gasoline or diesel product, although oil product forms different features and carried out segmental machining after having utilized cutting, enter raw material open loop degree of saturation before catalytic cracking still lower, for increasing gasoline, difficulty is large and quality is also relatively on the low side.
CN1955257A has introduced a kind of method of high-output qulified industrial chemicals, is mainly catalysis catalytic cracking diesel oil inferior and hydrogenating materials are mixed in proportion, and then produces catalytic reforming raw material and quality steam cracking ethylene preparation raw material by controlling reaction conditions.Although can process catalytic cracking poor ignition quality fuel, significantly increase the processing approach of inferior raw material and be converted into quality products, but still belong in hydrogenation process and transformed, failed and the mating of catalytic cracking process, catalytic cracking unit is not had to benifit simultaneously yet.
Summary of the invention
The problem existing for prior art, the technical problem to be solved in the present invention is to provide a kind of hydrocracking method of processing poor ignition quality fuel raw material.The method is carried out conventional catalytic diesel oil after the MCI reaction of not chain rupture of open loop, be not in harmonious proportion as diesel product, but return catalytic cracking unit as catalysis charging recirculation after Aromatics Extractive Project, can be by the high-octane rating that is converted into of this part diesel product maximum, the catalytic gasoline product of high added value, meet on the basis of processing poor ignition quality fuel raw material, improved to greatest extent the yield of gasoline of catalytic unit.
The invention provides a kind of combined technical method of processing poor ignition quality fuel, comprise the steps:
A) under hydrogenation modifying process condition, poor ignition quality fuel component mix with hydrogen after by the hydro-upgrading reaction zone of containing catalyst for hydro-upgrading bed;
B) step a) gained reaction effluent carries out gas-liquid separation, and gained product liquid enters aromatic extraction unit and carries out aromatic hydrocarbons separation, obtains non-aromatic raffinating oil and aromatic component; The non-aromatic component of raffinating oil obtaining can be used as high added value diesel product and is in harmonious proportion or carries out secondary processing; The aromatic component obtaining can enter catalytic cracking unit;
C) after the aromatic component of step b) gained mixes with conventional catalytically cracked material, enter catalytic cracking unit, under catalytic cracking cracking processing condition, carry out catalytic cracking reaction, and obtain gas, catalytic gasoline, catalytic diesel oil and mink cell focus through separation and fractionation;
According to combined technical method of the present invention, wherein also comprise step d), step c) gained catalytic diesel oil loops back step a) to be mixed with poor ignition quality fuel component, using as hydro-upgrading reaction feed.
The final boiling point of the poor ignition quality fuel component described in step a) is generally 330～400 ℃, and preferably 350～380 ℃, aromaticity content generally, more than 30 wt%, is preferably 40～90 wt%;
The nitrogen content of described diesel raw material, below 2000 μ g/g, is generally 50～1200 μ g/g, most preferably is 100～500 μ g/g.If the organonitrogen too high levels in diesel raw material, if nitrogen content is at 2000 μ g/g when above, can, before diesel raw material is by the hydro-upgrading reaction zone of containing catalyst for hydro-upgrading bed, by a hydrofining or hydrodenitrogenation catalyst bed, carry out part denitrogenation in advance.
The general secondary processing diesel oil of described inferior raw material, for example, can be selected from the processing catalytic diesel oil that obtains of middle-eastern crude or plant a kind of in coker gas oil or two kinds, can be specifically the secondary processing diesel oil component that processing Iran crude, the former wet goods of Saudi Arabia obtain.
The operational condition of the hydro-upgrading reaction zone described in step a) is: reaction pressure 6.0～12.0 MPa, and hydrogen to oil volume ratio 200: 1～1000: 1, volume space velocity is 0.1～5.0 h
-1, 260 ℃～455 ℃ of temperature of reaction; Preferred operational condition is reaction pressure 7.0～10.0 MPa, hydrogen to oil volume ratio 300: 1～900: 1, volume space velocity 1.0～3.0 h
-1, 300 ℃～400 ℃ of temperature of reaction.
Catalyst for hydro-upgrading described in step a) is the hydrogenation conversion catalyst containing molecular sieve, refers to general hydrocracking catalyst or is exclusively used in hydrogenation conversion catalyst of the present invention.Described catalyst for hydro-upgrading comprises hydrogenation active metals, molecular sieve component and alumina supporter.General hydrocracking catalyst comprises the hydrogenation active metals components such as Wo, Mo, Co, Ni, Fe, molecular sieve component and alumina supporter, and take the weight of catalyzer as benchmark, the content of hydrogenation component is 5%～40%.Being exclusively used in catalyst for hydro-upgrading of the present invention is to comprise by weight WO
3(or MoO
3) 13～25wt%, NiO (or CoO) 3～10wt%, molecular sieve 5～30wt% and aluminum oxide 5-30wt%, wherein molecular sieve can be Y type, β type or ZSM type molecular sieve.Conventional catalyst for hydro-upgrading can be selected existing various commercial catalysts, the catalyzer such as 3963 catalyzer, FC-18 catalyzer that such as FRIPP develops.Also can prepare specific catalyst for hydro-upgrading by the general knowledge of this area as required.
In step a), Hydrobon catalyst bed, except containing catalyst for hydro-upgrading bed, can also be contained in described hydro-upgrading reaction zone, and described Hydrobon catalyst bed is preferably disposed on the upstream of catalyst for hydro-upgrading bed.In the time that the nitrogen content in stock oil is too high, can carry out hydrofining by the Hydrobon catalyst bed arranging, so that it meets the charging demand of hydro-upgrading reaction.Described Hydrobon catalyst comprises the hydrogenation metal of carrier and institute's load.Take the weight of catalyzer as benchmark, Hydrobon catalyst generally includes metal component of group VIB in the periodic table of elements, counts 10%～35% as tungsten and/or molybdenum with oxide compound, is preferably 15%～30%; Group VIII metal counts 1%～7% as nickel and/or cobalt with oxide compound, is preferably 1.5%～6%.Carrier is inorganic refractory oxide, is generally selected from aluminum oxide, amorphous silicon aluminium, silicon-dioxide, titanium oxide etc.Described Hydrobon catalyst can be selected conventional pretreating catalyst by hydrocracking, wherein conventional pretreating catalyst by hydrocracking can be selected existing various commercial catalysts, such as Fushun Petrochemical Research Institute (FRIPP) develop 3936,3996, the hydrotreating catalyst such as FF-16, FF-26, FF-36; Also can be prepared by the general knowledge of this area as required.
Aromatics Extractive Project described in step b) also claims aromatic hydrocarbons extraction, it is the Liquid-liquid Extraction Processes with extraction agent aromatics separation from hydrocarbon mixture, can adopt the solvent extraction process of current industrial widespread use, in extraction tower, react, utilize aromatic hydrocarbons and the non-aromatics different solubility in different solvents to be separated, different being separated of boiling point that then recycles solvent and aromatic hydrocarbons, generally comprises extracting, solvent recuperation and three parts of solvent reclamation; Conventional extraction solvent has tetraethylene glycol, tetramethylene sulfone etc.
The operational condition of the Aromatics Extractive Project flow process extracting part extraction tower described in step b) is: tower internal pressure is 5～10 normal atmosphere, and temperature is 100～150 ℃, solvent ratio 10～20, reflux ratio 1.0～1.5; Preferred operational condition is 7～9 normal atmosphere of tower internal pressure, and temperature is 125～140 ℃, solvent ratio 14～16, reflux ratio 1.1～1.4.
Conventional catalytically cracked material initial boiling point described in step c) is generally 250～600 ℃, preferably 280～500 ℃.Generally being selected from the various heavy distillates that obtain of processing crude oil, as one or several in decompressed wax oil oil, wax tailings, long residuum, vacuum residuum, can be the above-mentioned heavy distillate that any crude oil of processing obtains.
Catalytic cracking unit described in step c) generally comprises three parts, reaction-regeneration system, fractionating system and absorption-stable system, the operational condition of its reaction-regeneration system is: reaction pressure 0.1～0.6 MPa, 400 ℃～650 ℃ of temperature of reaction, agent oil quality ratio is 3.0～8.0, and the reaction times is 1～10s; Preferred operational condition is reaction pressure 0.2～0.4MPa, 450 ℃～600 ℃ of temperature of reaction; Agent oil quality ratio is 4.0～7.0, and the reaction times is 2～6s.
Catalytic cracking catalyst described in step c) is the conventional catalytic cracking catalyst of this area.Described catalytic cracking catalyst generally comprises molecular sieve and carrier, and its molecular sieve content is about 5～15%, can be X-type or Y zeolite; The composition of carrier has natural clay, synthetic low manosil AS aluminium or high aluminum silicate.
Compared with prior art, poor ignition quality fuel combination technological method for processing of the present invention has the following advantages:
1, the higher poor ignition quality fuel of processing aromaticity content, after hydro-upgrading selective opening, is converted into alkylbenzene by dicyclo and the above aromatic hydrocarbons of dicyclo, then after Aromatics Extractive Project separates, enters catalytic cracking unit, can increase the output of catalytically cracked gasoline; Product after hydrogenation is as catalytically cracked material simultaneously, can reduce the sulphur content in catalyst article, in addition according to the mechanism of catalyzed reaction, the increase of monocycle alkylbenzene in raw material, after catalytic cracking, the octane value of gained catalytic gasoline also has certain amplification; The catalytic diesel oil inferior that catalytic unit generates can loop back this modifying apparatus and continue processing, for an economically viable circuit has been found in the processing of poor ignition quality fuel.Simultaneously through Aromatics Extractive Project generate raffinate oil in contain a large amount of paraffinic hydrocarbonss, there is the feature of low BMCI value and high hexadecane value, can be used as the preparing ethylene by steam cracking raw material of high-quality or the diesel oil blending component of high added value.
2, the inventive method is carried out degree of depth coupling by hydro-upgrading, Aromatics Extractive Project and catalytic cracking in technical process, on the basis of improving the quality of products, obtains desirable comprehensive process effect.In technical process, the inventive method is that different units is combined, and has the advantages such as saving equipment, process cost are low, the improvement of the heat-exchange system simultaneously bringing due to coupling, also reduced to a certain extent the energy consumption of installing, reduced investment, be with a wide range of applications.
Accompanying drawing explanation
Fig. 1 is the schematic flow sheet of processing method of the present invention.
Embodiment
Below in conjunction with accompanying drawing, combined technical method of the present invention is elaborated.In Fig. 1, just list out the main explanation of technical process, in schematic diagram, also omitted some necessary equipment and containers.
As shown in Figure 1, to process poor ignition quality fuel combination process flow process as follows in the present invention: poor ignition quality fuel raw material 1 enters hydroconversion reaction zone 3 after mixing with hydrogen 2, with hydrogenation catalyst contact reacts; Reaction effluent 4 enters separation system 5, gas phase 6 is discharged on top, and the liquid phase 7 that bottom obtains enters aromatic extraction unit 8, and gained is non-aromatic raffinates oil and 9 go out device, aromatic component 10 enters catalytic cracking unit 12 after mixing with conventional fcc raw material 11, reacts with catalytic cracking catalyst; Reaction effluent 13 enters separation column 14 and separates, and obtains successively gas phase 15, catalytic gasoline 16, catalytic diesel oil 17, mink cell focus 18 from top to bottom; Wherein catalytic diesel oil 17 loops back hydroconversion reaction zone and mixes with poor ignition quality fuel raw material.
Next by specific embodiment, combined technical method of the present invention is further described.
Embodiment 1
Adopt the combination process flow process shown in Fig. 1, select catalytic diesel oil to carry out hydrogenation production as poor ignition quality fuel raw material, product is mixed into catalytic cracking unit with catalytic cracking charging after by Aromatics Extractive Project.The catalyzer using in embodiment is commercial catalyst FF-36 hydrotreating catalyst, 3963 catalyst for hydro-upgrading and LHO-1 catalytic cracking catalyst.
Raw material oil properties is in table 1, and operational condition is in table 2.
Adopt the combination process flow process shown in Fig. 1, select coker gas oil to carry out hydrogenation production as poor ignition quality fuel raw material, product is mixed into catalytic cracking unit with catalytic cracking charging after by Aromatics Extractive Project.The catalyzer using in embodiment is with embodiment 1.
Raw material oil properties is in table 1, and operational condition is in table 2.
Feedstock property in the listed embodiment 1 and 2 of table 1 is hydrogenation unit poor ignition quality fuel feed properties, and in its combination process, the conventional charging of catalytic cracking unit is identical with charging in comparative example 1.
Comparative example 1
Comparative example 1 is the technological process of catalyzed cracking processing heavy feed stock.Table 3 is the contrast of processing different material catalytic gasoline character.
Table 1 stock oil property list.
| ? | Embodiment 1 | |
Comparative example 1 |
| Raw material sources | Catalytic diesel oil | Coker gas oil | Decompressed wax oil |
| Density (20 ℃)/gcm -3 | 0.9543 | 0.8763 | 0.9295 |
| Boiling range scope/℃ | 160～375 | 167～370 | 355～595 |
| Sulphur/μ gg -1 | 12000 | 11200 | 16000 |
| Nitrogen/μ gg -1 | 890 | 130 | 1600 |
| Aromaticity content/% | 78.7 | 41.3 | 48.8 |
Table 2 reaction conditions.
| ? | Embodiment 1 | |
Comparative example 1 |
| Hydro-upgrading | ? | ? | ? |
| Catalyzer | FF-36/3963 | FF-36/3963 | --- |
| Reaction pressure/MPa | 8.0 | 8.0 | --- |
| Average reaction temperature/℃ | 339/364 | 330/359 | --- |
| LHSV/h -1 | 1.0 | 1.0 | --- |
| Hydrogen to oil volume ratio | 800∶1 | 800∶1 | --- |
| |
12 | 4 | --- |
| Aromatics Extractive Project | ? | ? | ? |
| Solvent | Tetramethylene sulfone | Tetramethylene sulfone | --- |
| |
15 | 15 | --- |
| Extraction temperature/℃ | 135 | 135 | --- |
| Extracting pressure/MPa | 0.7 | 0.7 | --- |
| The BMCI value of raffinating oil | 5.3 | 4.8 | --- |
| Catalytic cracking | ? | ? | ? |
| Pressure/MPa | 0.18 | 0.18 | 0.18 |
| Temperature of reaction/℃ | 540 | 535 | 533 |
| Agent weight of oil ratio | 5.4 | 5.4 | 5.4 |
| Reaction times, s | 2.5 | 2.5 | 2.5 |
| Poor ignition quality fuel/decompressed wax oil | 1:3 | 1:3 | — |
Table 3 catalytic gasoline main character.
| Raw material sources | Embodiment 1 | |
Comparative example 1 |
| Yield of gasoline/% | 60 | 56 | 53 |
| Content of sulfur in gasoline/μ gg -1 | 320 | 500 | 800 |
| Gasoline octane rating/MON | 84 | 81 | 79 |
Can be found out by above-mentioned example, adopt the inventive method to process poor ignition quality fuel raw material, compared with comparative example, in yield of gasoline and sulphur content, have very large advantage, can process catalytic diesel oil inferior, improve added value of product, there is certain practicality simultaneously.
Can find out from above embodiment and comparative example, after hydro-upgrading selective opening, dicyclo and the above aromatic hydrocarbons of dicyclo are converted into alkylbenzene, again after Aromatics Extractive Project separates, enter catalytic cracking unit, can utilize the feature of catalyzed reaction after alkylbenzene chain rupture, to be enriched in gasoline component, increase output and the octane value of catalytically cracked gasoline; Reduce the sulphur content in catalyst article simultaneously; Through Aromatics Extractive Project generate raffinate oil in contain a large amount of paraffinic hydrocarbonss, there is the feature of low BMCI value and high hexadecane value, can be used as the preparing ethylene by steam cracking raw material of high-quality or the diesel oil blending component of high added value.
In technical process, hydro-upgrading, Aromatics Extractive Project and catalytic cracking are carried out to degree of depth coupling, on the basis of improving the quality of products, obtain desirable comprehensive process effect, there is the advantages such as saving equipment, process cost is low, the improvement of the heat-exchange system simultaneously bringing due to coupling, also reduced to a certain extent the energy consumption of installing, reduced investment, be with a wide range of applications.
Claims (12)
1. a combined technical method of processing poor ignition quality fuel, comprises the steps:
A) under hydrogenation modifying process condition, poor ignition quality fuel component mix with hydrogen after by the hydro-upgrading reaction zone of containing catalyst for hydro-upgrading bed;
B) step a) gained reaction effluent carries out gas-liquid separation, and gained product liquid enters aromatic extraction unit and carries out aromatic hydrocarbons separation, obtains non-aromatic raffinating oil and aromatic component;
C) after the aromatic component of step b) gained mixes with conventional catalytically cracked material, enter catalytic cracking unit, under catalytic cracking cracking processing condition, carry out catalytic cracking reaction, and obtain gas, catalytic gasoline, catalytic diesel oil and mink cell focus through separation and fractionation.
2. in accordance with the method for claim 1, it is characterized in that, also comprise step d), step c) gained catalytic diesel oil loops back step a), after mixing with poor ignition quality fuel component as hydro-upgrading reaction feed.
3. in accordance with the method for claim 1, it is characterized in that, the final boiling point of described poor ignition quality fuel component is 330～400 ℃, and aromaticity content is more than 30%wt%, and nitrogen content is below 2000 μ g/g.
4. in accordance with the method for claim 1, it is characterized in that, described poor ignition quality fuel is selected from the processing catalytic diesel oil that obtains of middle-eastern crude or plants a kind of in coker gas oil or two kinds.
5. in accordance with the method for claim 1, it is characterized in that, the operational condition of the hydro-upgrading reaction zone described in step a) is: reaction pressure 6.0～12.0 MPa, and hydrogen to oil volume ratio 200: 1～1000: 1, volume space velocity is 0.1～5.0 h
-1, 260 ℃～455 ℃ of temperature of reaction.
6. in accordance with the method for claim 1, it is characterized in that, described catalyst for hydro-upgrading comprises WO by weight
3or MoO
313～25wt%, NiO or CoO 3～10wt%, molecular sieve 5～30wt% and aluminum oxide 5-30wt%, wherein molecular sieve is Y type, β type or ZSM type molecular sieve.
7. in accordance with the method for claim 1, it is characterized in that, Hydrobon catalyst bed is also contained in described hydro-upgrading reaction zone, and described Hydrobon catalyst bed is preferably disposed on the upstream of catalyst for hydro-upgrading bed.
8. in accordance with the method for claim 1, it is characterized in that, the operational condition of the Aromatics Extractive Project flow process extracting part extraction plant described in step b) is: tower internal pressure is 5～10 normal atmosphere, and temperature is 100～150 ℃, solvent ratio 10～20, reflux ratio 1.0～1.5.
9. in accordance with the method for claim 1, it is characterized in that, described solvent is tetraethylene glycol or tetramethylene sulfone.
10. in accordance with the method for claim 1, it is characterized in that, conventional catalytically cracked material initial boiling point described in step c) is 250～600 ℃, and catalytically cracked material is selected from one or several in processing the crude oil decompressed wax oil, wax tailings, long residuum or the vacuum residuum that obtain.
11. in accordance with the method for claim 1, it is characterized in that, the processing condition of catalytic cracking reaction are described in step c): reaction pressure 0.1～0.6 MPa, 400 ℃～650 ℃ of temperature of reaction, agent-oil ratio is 4～7, duration of contact 2～6s.
12. in accordance with the method for claim 1, it is characterized in that, the non-aromatic component of raffinating oil of step b) gained is as diesel product blend component.
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| CN106753552A (en) * | 2017-01-22 | 2017-05-31 | 中石化炼化工程（集团）股份有限公司 | A kind of method that utilization catalytic cracking diesel oil produces high-knock rating gasoline |
| CN106753551A (en) * | 2017-01-22 | 2017-05-31 | 中石化炼化工程（集团）股份有限公司 | A kind of method that utilization catalytic cracking diesel oil produces high-knock rating gasoline |
| CN108102704A (en) * | 2016-11-24 | 2018-06-01 | 中国石油化工股份有限公司 | A kind of method for producing premium |
| CN110437875A (en) * | 2019-08-31 | 2019-11-12 | 中海油天津化工研究设计院有限公司 | A kind of catalytic cracking diesel oil hydroisomerizing-deep catalytic cracking technology |
| CN112779050A (en) * | 2019-11-11 | 2021-05-11 | 中国石油天然气股份有限公司 | Processing method of poor-quality catalytic diesel oil |
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| CN112779050A (en) * | 2019-11-11 | 2021-05-11 | 中国石油天然气股份有限公司 | Processing method of poor-quality catalytic diesel oil |
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