CN114763489B - Catalytic diesel oil combined treatment process and treatment system - Google Patents
Catalytic diesel oil combined treatment process and treatment system Download PDFInfo
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- 238000011282 treatment Methods 0.000 title claims abstract description 64
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- 238000006243 chemical reaction Methods 0.000 claims abstract description 85
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- 238000005194 fractionation Methods 0.000 claims abstract description 28
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- 238000000926 separation method Methods 0.000 claims abstract description 20
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- 239000003054 catalyst Substances 0.000 claims description 51
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- 239000012071 phase Substances 0.000 claims description 16
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- 238000011284 combination treatment Methods 0.000 claims description 11
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- 238000000605 extraction Methods 0.000 claims description 9
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- NJMWOUFKYKNWDW-UHFFFAOYSA-N 1-ethyl-3-methylimidazolium Chemical compound CCN1C=C[N+](C)=C1 NJMWOUFKYKNWDW-UHFFFAOYSA-N 0.000 claims description 2
- FXHOOIRPVKKKFG-UHFFFAOYSA-N N,N-Dimethylacetamide Chemical compound CN(C)C(C)=O FXHOOIRPVKKKFG-UHFFFAOYSA-N 0.000 claims description 2
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- 229910052751 metal Inorganic materials 0.000 description 7
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- 150000002431 hydrogen Chemical class 0.000 description 6
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- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- 125000002619 bicyclic group Chemical group 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
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- 150000001924 cycloalkanes Chemical class 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
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- 239000000463 material Substances 0.000 description 1
- AUHZEENZYGFFBQ-UHFFFAOYSA-N mesitylene Substances CC1=CC(C)=CC(C)=C1 AUHZEENZYGFFBQ-UHFFFAOYSA-N 0.000 description 1
- 125000001827 mesitylenyl group Chemical group [H]C1=C(C(*)=C(C([H])=C1C([H])([H])[H])C([H])([H])[H])C([H])([H])[H] 0.000 description 1
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Classifications
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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
- C10G67/00—Treatment of hydrocarbon oils by at least one hydrotreatment process and at least one process for refining in the absence of hydrogen only
-
- 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
- C10G2300/00—Aspects relating to hydrocarbon processing covered by groups C10G1/00 - C10G99/00
- C10G2300/40—Characteristics of the process deviating from typical ways of processing
- C10G2300/4006—Temperature
-
- 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
- C10G2300/00—Aspects relating to hydrocarbon processing covered by groups C10G1/00 - C10G99/00
- C10G2300/40—Characteristics of the process deviating from typical ways of processing
- C10G2300/4012—Pressure
-
- 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
- C10G2300/00—Aspects relating to hydrocarbon processing covered by groups C10G1/00 - C10G99/00
- C10G2300/40—Characteristics of the process deviating from typical ways of processing
- C10G2300/4018—Spatial velocity, e.g. LHSV, WHSV
-
- 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
- C10G2300/00—Aspects relating to hydrocarbon processing covered by groups C10G1/00 - C10G99/00
- C10G2300/40—Characteristics of the process deviating from typical ways of processing
- C10G2300/44—Solvents
-
- 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
- C10G2300/00—Aspects relating to hydrocarbon processing covered by groups C10G1/00 - C10G99/00
- C10G2300/70—Catalyst aspects
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P30/00—Technologies relating to oil refining and petrochemical industry
- Y02P30/20—Technologies relating to oil refining and petrochemical industry using bio-feedstock
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- Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
Abstract
The invention discloses a catalytic diesel oil combined treatment process and a catalytic diesel oil combined treatment system, wherein the catalytic diesel oil combined treatment system comprises a pretreatment unit, a pretreatment agent recovery unit, a fractionation unit, a first boiling bed hydrogenation reaction zone, a second boiling bed hydrogenation reaction zone and a separation unit; the catalytic diesel oil is treated by the system to obtain a light fraction product taking monocyclic aromatic hydrocarbon as a main component. The method solves the technical problems of strong heat release, easy hot spot generation, difficult control of reaction process, poor product quality, low yield and short device operation period in the hydrogenation conversion process caused by high aromatic hydrocarbon content and complex composition and large difference of hydrogenation conversion rules of the catalytic diesel, realizes reasonable and efficient conversion of each component of the catalytic diesel, greatly reduces hydrogen consumption, remarkably improves the quality and yield of high value-added aromatic hydrocarbon products, improves long-period operation of the device, and greatly promotes quality improvement and efficiency improvement of a refinery.
Description
Technical Field
The invention belongs to the technical field of petrochemical industry, and particularly relates to a high-efficiency conversion process for catalyzing diesel oil.
Background
The catalytic cracking technology is one of the most important technical means for heavy oil conversion, and plays an important role in the oil refining industry. However, refineries face many problems in processing poor catalytic diesel oil, especially the aromatic hydrocarbon content is as high as 60%. The hydrogenation technology of poor quality and high aromatic hydrocarbon catalytic diesel oil can be divided into hydrogenation refining technology, hydrogenation modification technology, hydrocracking technology and hydrogenation conversion technology according to different production purposes. The hydrofining technology mainly comprises MQD (Maximum quality distillation) combined refining technology of UOP company, synSat process technology, prime-D hydrogenation technology developed by Axens, REDAR catalyst and process technology and the like, and the technical difficulties of processing and utilization are that the catalytic diesel oil has high sulfur content, high density and low cetane numberIn order to deeply desulfurize and deeply remove arene to improve the cetane number, a diesel oil product meeting the quality requirement is difficult to produce by adopting a common diesel oil hydrofining technology. The hydro-upgrading technology mainly means that polycyclic aromatic hydrocarbon in diesel oil is subjected to hydro-saturation through a hydro-processing method to achieve the purposes of reducing the density of the diesel oil and improving the cetane number of the diesel oil, and mainly comprises an MAK-LCO hydro-upgrading process, a Denmark Tops @ 632e two-stage hydrogenation process, a NEBULA technology and an ASAT technology. Hydrocracking technology is the main technology of deep processing of heavy oil, and a hydrocracking device and the hydrocracking technology can be configured in various ways. The hydrocracking technology which is developed abroad in recent years and is characterized by processing catalytic diesel mainly comprises a HyCycycle Unicracking process, an APCU process and the like. Hydroconversion technology LCO Unicracking of the UOP company TM Techniques and LCO-X TM The FD2G technology of FRIPP in medium and petrochemical industry mainly converts catalytic diesel oil into gasoline blending components with high octane number or BTX chemical raw materials by hydrogenation. The four process routes all have the problems of no load requirement of product indexes, high hydrogen consumption and poor economy caused by overhigh content of the naphthenic hydrocarbon in the product.
CN107286987A provides a combined process for treating poor diesel. Mixing the poor diesel oil raw material with hydrogen, then entering a fixed bed hydrogenation reaction zone, and carrying out hydrogenation reaction under the action of a hydrofining catalyst; and mixing the obtained reaction product oil with hydrogen, then feeding the mixture into a fluidized bed hydrocracking reaction zone, carrying out hydrocracking reaction in the presence of a fluidized bed hydrogenation conversion catalyst, and separating to obtain a product.
Disclosure of Invention
Aiming at the defects in the prior art, the invention aims to provide a catalytic diesel oil combined treatment process and a treatment system, wherein the treatment process separates different hydrocarbon components of the catalytic diesel oil from a molecular oil refining level, simultaneously matches a pretreatment, distillation and hydrogenation combined process, treats different types of aromatic hydrocarbons in the catalytic diesel oil according to respective proper reaction paths, solves the technical problems of strong heat release, easy hot spot generation, difficult control of reaction process, poor product quality and low yield and short device operation period in the hydrogenation conversion process caused by high content of the aromatic hydrocarbons in the catalytic diesel oil and large difference of complex hydrogenation conversion rules, realizes reasonable and efficient conversion of the components of the catalytic diesel oil, greatly reduces hydrogen consumption, remarkably improves the quality and the yield of high value-added aromatic hydrocarbon products, has vital significance for ensuring long-period operation of the device, and greatly promotes quality improvement and efficiency of a refinery.
The invention provides a catalytic diesel oil combined treatment process, which comprises the following steps:
(1) The catalytic diesel enters a pretreatment unit, contacts with a pretreatment agent and is separated to obtain an aromatic hydrocarbon-rich component and an alkane-rich component;
(2) Separating the aromatic hydrocarbon-rich component obtained in the step (1) to obtain aromatic hydrocarbon fraction and a regenerated pretreating agent;
(3) The aromatic hydrocarbon fraction obtained in the step (2) enters a fractionation unit, and a first gas phase, a light fraction, a middle fraction and a heavy fraction are obtained after separation;
(4) The heavy fraction obtained in the step (3) enters a first boiling bed hydrogenation reaction zone, and is subjected to hydrogenation reaction under the action of a first hydrogenation catalyst and hydrogen to generate a first reaction effluent;
(5) And (3) feeding the intermediate fraction obtained in the step (3) and the first reaction effluent obtained in the step (4) into a second fluidized bed hydrogenation reaction zone, reacting under the action of a second hydrogenation catalyst and hydrogen to generate a second reaction effluent, carrying out gas-liquid separation on the second reaction effluent to obtain a second gas phase and a liquid phase, and feeding the obtained liquid phase into the fractionation unit in the step (3) for treatment.
In the combined treatment process of the catalytic diesel oil, the aromatic hydrocarbon content in the catalytic diesel oil in the step (1) is higher than 50wt%, and preferably 55wt% -80 wt%.
In the catalytic diesel oil combined treatment process, the pretreatment agent in the step (1) can be at least one selected from sulfone compounds, aldehyde compounds, alkanone compounds, amide compounds and ionic liquids, and is preferably a sulfone compound; the pretreating agent can be sulfolane, N-methylpyrrolidone, N-dimethylacetamide, caprolactam, [ emim]N(CN)2、[3-mebupy]N(CN) 2 At least one of (a).
In the catalytic diesel oil combined treatment process, the operation conditions of the pretreatment unit in the step (1) are as follows: the temperature is 30-200 ℃, preferably 30-180 ℃, and the mass ratio of the pretreating agent to the catalytic diesel oil is 0.5-25.0, preferably 5.0-20.0.
In the catalytic diesel oil combined treatment process, the cutting temperature of the light fraction and the middle fraction in the step (1) is 150-250 ℃, and preferably 180-220 ℃; the cutting temperature of the middle fraction and the heavy fraction is 260-320 ℃, and preferably 290-310 ℃.
In the catalytic diesel oil combined treatment process, the light fraction in the step (1) can be directly discharged from a device as a product, and the light fraction mainly comprises a C5-C9 monocyclic aromatic hydrocarbon component, and specifically can comprise light aromatic hydrocarbons such as benzene, toluene, xylene, methyl ethylbenzene, mesitylene and the like.
In the catalytic diesel oil combined treatment process, the first fluidized bed hydrogenation reaction zone can be provided with more than one fluidized bed reactor, preferably a fluidized bed reactor with a three-phase separator arranged in the reactor is adopted, and particularly a fluidized bed reactor with a three-phase separator developed by the petrochemical research institute of China petrochemical company Limited can be adopted.
In the catalytic diesel oil combined treatment process, the second fluidized bed hydrogenation reaction zone can be provided with more than one fluidized bed reactor, preferably a fluidized bed reactor with a three-phase separator arranged in the reactor is adopted, and particularly a fluidized bed reactor with a three-phase separator developed by the petrochemical research institute of China petrochemical company Limited can be adopted.
In the catalytic diesel oil combined treatment process, the first hydrogenation catalyst and the second hydrogenation catalyst filled in the first fluidized bed hydrogenation reaction zone and the second fluidized bed hydrogenation reaction zone may be the same or different, and preferably, the second hydrogenation catalyst used in the second fluidized bed hydrogenation reaction zone is discharged to the first fluidized bed hydrogenation reaction zone to be used as the first hydrogenation catalyst.
In the above catalytic diesel oil combined treatment process, the first hydrogenation catalyst and the second hydrogenation catalyst may be the existing diesel oil hydrogenation catalysts in the field, or may be prepared by themselves according to the methods disclosed in the prior art. Specifically, in the invention, the first hydrogenation catalyst and the second hydrogenation catalyst are preferably prepared by using high-silicon aluminum oxide and a molecular sieve as carriers, using VIII group metal and VIB group metal as active metal components, and taking the weight of the catalyst as a reference, the content of the high-silicon aluminum oxide is 30-70%, the content of the molecular sieve is 10-50%, the content of the VIII group metal is 1-9% by oxide, and the content of the VIB group metal is 10-30% by oxide. The group VIII metal is preferably Ni and/or Co; the group VIB metal is preferably W and/or Mo; the molecular sieve is selected from one or more of Y-type molecular sieve, beta molecular sieve, ZSM-5 molecular sieve, SAPO molecular sieve and MCM-41 mesoporous molecular sieve.
In the catalytic diesel oil combined treatment process, the alkane-rich component obtained in the step (1) can be returned to a catalytic cracking device for treatment, and can also be used as a raw material for preparing olefin by using devices such as steam cracking devices, catalytic cracking devices and the like.
In the catalytic diesel oil combined treatment process, the process conditions of the first boiling bed hydrogenation reaction zone in the step (4) are as follows: the reaction temperature is 350-450 ℃, the preferential temperature is 380-440 ℃, the reaction pressure is 5.0-15.0 MPa, the preferential pressure is 8.0-18.0 MPa, the volume ratio of hydrogen to oil is 500-2000, the preferential pressure is 600-1500, and the liquid hourly space velocity is 0.1-5.0 h -1 Preferably 0.2 to 2.0h -1 。
In the catalytic diesel oil combined treatment process, the process conditions of the second fluidized bed hydrogenation reaction zone in the step (5) are as follows: the reaction temperature is 350-450 ℃, preferably 380-440 ℃, the reaction pressure is 5.0-15.0 MPa, preferably 8.0-18.0 MPa, the volume ratio of hydrogen to oil is 500-2000, preferably 600-1500, and the liquid hourly space velocity is 0.1-5.0 h -1 Preferably 0.2 to 2.0h -1 。
In the catalytic diesel oil combined treatment process, the reaction temperature of the second boiling bed hydrogenation reaction zone in the step (5) is 5-30 ℃ higher than that of the first boiling bed hydrogenation reaction zone in the step (4), and preferably 5-15 ℃ higher.
In a second aspect the present invention provides a catalytic diesel fuel combination treatment system, the combination treatment system comprising:
the pretreatment unit is used for receiving and treating catalytic diesel and a pretreatment agent to obtain a component rich in alkane and a component rich in aromatic hydrocarbon after treatment;
the pretreatment agent recovery unit is used for receiving the aromatic-rich component from the pretreatment unit, and after separation, an aromatic fraction and a regenerated pretreatment agent are obtained, and the regenerated pretreatment agent returns to the pretreatment unit for recycling;
the fractionation unit is used for receiving and processing the aromatic hydrocarbon fraction from the pretreatment agent recovery unit, and separating to obtain a light fraction, a middle fraction and a heavy fraction;
the first ebullated bed hydrogenation reaction zone is used for receiving the heavy fraction from the fractionation unit and reacting the heavy fraction under the action of hydrogen and a first hydrogenation catalyst to obtain a first reaction effluent;
and the second boiling bed hydrogenation reaction zone is used for receiving the first reaction effluent from the first boiling bed hydrogenation reaction zone and the middle fraction from the fractionation unit, reacting under the action of hydrogen and the first hydrogenation catalyst to obtain a second reaction effluent, treating the second reaction effluent in the separation unit, and treating the liquid phase obtained after separation in the fractionation unit.
In the above catalytic diesel oil combined treatment system, the pretreatment unit may be implemented by a solvent refining device or an aromatic hydrocarbon extraction device.
In the above catalytic diesel oil combined treatment system, the first fluidized bed hydrogenation reaction zone may be provided with more than one fluidized bed reactor, preferably a fluidized bed reactor in which a three-phase separator is disposed inside the reactor, and specifically a fluidized bed reactor with a three-phase separator developed by the institute of petrochemical engineering, france, of the china petrochemical company ltd.
In the above catalytic diesel oil combined treatment system, the second fluidized bed hydrogenation reaction zone may be provided with more than one fluidized bed reactor, preferably a fluidized bed reactor in which a three-phase separator is disposed inside the reactor, and specifically a fluidized bed reactor with a three-phase separator developed by the institute of petrochemical engineering, france, of the china petrochemical company ltd.
In the above catalytic diesel combined treatment system, the separation unit comprises a gas-liquid separator and an optional fractionating tower; the gas-liquid separator may comprise a high-pressure separator and a low-pressure separator, and the fractionating tower may be a fractionating tower existing in the field, and specifically may be a plate tower or a packed tower.
Compared with the prior art, the catalytic diesel oil combined treatment process and the catalytic diesel oil combined treatment system have the following advantages:
1. in the catalytic diesel oil combined treatment process, based on the concept of molecular oil refining, physical separation (pretreatment and distillation) and chemical conversion (boiling bed hydrogenation) are organically combined, different types of molecules are subjected to zone reaction according to ideal controllable reaction paths of the molecules, the aim of ' alkene is suitable for olefin and ' arene is suitable for aromatic hydrocarbon ' is fulfilled, alkane and arene in catalytic diesel oil are respectively converted, alkane and cycloalkane and other alkane-rich components are used as raw materials of a catalytic cracking device for converting to generate alkene, and bicyclic and polycyclic aromatic hydrocarbon are directionally hydrogenated to convert monocyclic aromatic hydrocarbon components with high added value mainly BTX to the maximum extent.
2. In the catalytic diesel oil combined treatment process, the first fluidized bed hydrogenation reaction zone and the second fluidized bed hydrogenation reaction zone adopt a fluidized bed hydrogenation technology, and the temperature and the pressure in a reaction space are the same by utilizing the full back-mixing characteristic of the fluidized bed hydrogenation technology, so that the control of a reaction path is facilitated; meanwhile, for a high aromatic hydrocarbon heat release system such as catalytic diesel oil, the generation of hot spots can be effectively avoided.
3. In the catalytic diesel oil combined treatment process, the first reaction effluent with higher temperature generated in the first boiling bed hydrogenation reaction zone and the middle distillate with lower temperature from the fractionation unit are mixed and enter the second boiling bed hydrogenation reaction zone, so that the condition that the second boiling bed hydrogenation reaction zone has hot spots can be reduced, the cold hydrogen consumption can be greatly reduced, the operation cost is reduced, and the economy of the whole process is improved. The higher temperature liquid phase produced in the second ebullated bed hydrogenation reaction zone is mixed with the lower temperature aromatic components from the pretreatment unit, which greatly reduces the heat requirement of the fractionation unit.
4. In the catalytic diesel oil combined treatment process, a second hydrogenation catalyst with higher activity is used in a second boiling bed hydrogenation reaction zone, the zone mainly generates a hydrocracking reaction of bicyclic aromatic hydrocarbons, the feed components of the reaction zone are lighter, the coking rate under high-temperature reaction is relatively lower, meanwhile, the catalyst is stronger in acidity and high in cracking effect, the activity of the catalyst is reduced after the catalyst is used for a period of time, and then the catalyst is discharged into the first boiling bed hydrogenation reaction zone for utilization, so that the gradient utilization of the catalyst is realized, the coking tendency of polycyclic aromatic hydrocarbons in the feed of the first boiling bed hydrogenation reaction zone at high temperature can be effectively reduced, the excessive hydrogenation saturation of the polycyclic aromatic hydrocarbons is relieved, and the controllable conversion of the polycyclic aromatic hydrocarbons hydrogenation process is realized.
5. In the catalytic diesel combined treatment system, through the combined processes of pretreatment, fractionation and hydrogenation, the fractionation unit not only plays a role in separating the feeding materials of the subsequent first fluidized bed hydrogenation reaction zone and the second fluidized bed hydrogenation reaction zone, but also can reduce the liquid phase separation obtained by the second fluidized bed hydrogenation reaction zone to obtain a target product, and seems to be obtained only by replacing the position of the fractionation tower, but a good technical effect is brought, one fractionation tower can be omitted, and the investment and operation cost of the device is greatly reduced.
Drawings
FIG. 1 is a schematic diagram of a combined treatment process and treatment system for catalytic diesel fuel.
Detailed Description
The technical features of the present invention will be further described by way of examples with reference to the accompanying drawings, but the present invention is not limited to these examples.
As shown in figure 1, the invention provides a catalytic diesel oil combined treatment process, wherein catalytic diesel oil 1 enters a pretreatment unit 2, contacts with a pretreatment agent 4 and is separated to obtain an aromatic hydrocarbon-rich component 6 and an alkane-rich component 5; the obtained aromatic hydrocarbon-rich component enters a pretreatment agent recovery unit 3, and is separated to obtain an aromatic hydrocarbon fraction 7 and a regeneration pretreatment agent 8, wherein the regeneration pretreatment agent 8 can be recycled to be used by the pretreatment unit; the obtained aromatic hydrocarbon fraction 7 enters a fractionation unit 9, and a first gas phase 24, a light fraction 10, a middle fraction 11 and a heavy fraction 12 are obtained after separation; wherein, the heavy fraction 12 and hydrogen 14 enter a first boiling bed hydrogenation reaction zone 13, and are subjected to hydrogenation reaction under the action of a first hydrogenation catalyst and hydrogen to generate a first reaction effluent 15; the obtained first reaction effluent 15, the middle distillate 11 and the hydrogen 14 enter a second ebullated bed hydrogenation reaction zone 16, react under the action of a second hydrogenation catalyst and the hydrogen to generate a second reaction effluent 17, the second reaction effluent 17 enters a separation unit, the separation unit comprises a high-pressure separator 18 and a low-pressure separator 19, gas 20 and a liquid phase 21 are obtained after separation of the high-pressure separator, the liquid phase 21 further enters the low-pressure separator 19 to be separated to obtain a dry gas 22 and a liquid phase 23, and the obtained liquid phase 23 enters a fractionation unit 9 to be circularly treated.
The basic properties of the catalytic diesel fuels used in the examples according to the invention and in the comparative examples are shown in Table 1.
TABLE 1 basic Properties of catalytic Diesel
Example 1
In the embodiment, the process flow shown in fig. 1 is adopted, and catalytic diesel enters a pretreatment unit, wherein the pretreatment unit is an aromatic hydrocarbon extraction device, an extracting agent is sulfolane, the extraction temperature is 170 ℃, and the mass ratio of the agent to the oil is 15.0; and (3) introducing the extracted aromatic-rich component into a fractionation unit, wherein the dry point temperatures of the light fraction and the middle fraction are 220 ℃ and 310 ℃ respectively. The first boiling bed reaction zone and the second boiling bed reaction zone adopt the same hydrogenation catalyst, the hydrogenation catalyst adopts FC-70 catalyst which is subjected to fragmentation treatment (is crushed into short strips with the diameter of 0.5-1.0 mm) and developed by the institute of petrochemical engineering, dalian of the China petrochemical industry, inc., and the petrochemical industry research institute, wherein the hydrogenation catalyst adopted by the second boiling bed reaction zone is the catalyst after the first boiling bed reaction zone operates for 3 months; the temperature of a hydrogenation reaction zone of the first boiling bed is 405 ℃, the reaction pressure is 10.0MPa, and the hydrogen oilThe liquid hourly space velocity is 1.2h and the ratio is 800 -1 (ii) a The temperature of a hydrogenation reaction zone of the second boiling bed is 420 ℃, the reaction pressure is 10.0MPa, the hydrogen-oil ratio is 800, and the liquid hourly volume space velocity is 0.6 h -1 (ii) a The specific test results are shown in Table 2.
Example 2
In the embodiment, the process flow shown in fig. 1 is adopted, catalytic diesel oil enters a pretreatment unit, wherein the pretreatment unit is set as an aromatic extraction device, an extracting agent is N-methylpyrrolidone, the extraction temperature is 150 ℃, and the mass ratio of the agent to the oil is 10.0; and (3) introducing the extracted aromatic-rich component into a fractionation unit, wherein the dry point temperatures of the light fraction and the middle fraction are 180 ℃ and 290 ℃ respectively. The first fluidized bed reaction zone and the second fluidized bed reaction zone adopt the same hydrogenation catalyst, and the hydrogenation catalyst is an FC-70 catalyst which is subjected to crushing treatment (is crushed into a short strip shape of 0.5-1.0 mm) and developed by the institute of petrochemical engineering, dalian, of the China petrochemical industry, inc.; the temperature of a hydrogenation reaction zone of the first boiling bed is 410 ℃, the reaction pressure is 12.0MPa, the hydrogen-oil ratio is 700, and the liquid hourly volume space velocity is 1.0 h -1 (ii) a The temperature of a hydrogenation reaction zone of the second boiling bed is 425 ℃, the reaction pressure is 12.0MPa, the hydrogen-oil ratio is 700, and the liquid hourly space velocity is 0.5 h -1 (ii) a The specific test results are shown in Table 2.
Example 3
Substantially the same as example 1, except that the extractant in the pretreatment unit is emim]N (CN) 2, the extraction temperature is 40 ℃, and the mass ratio of solvent to oil is 10; the extracted aromatic-rich component enters a fractionation unit, and the dry point temperatures of the light fraction and the middle fraction are 180 ℃ and 290 ℃ respectively. The first fluidized bed reaction zone and the second fluidized bed reaction zone adopt the same hydrogenation catalyst, and the hydrogenation catalyst is an FC-70 catalyst which is subjected to crushing treatment (crushed into short strips of 0.5-1.0 mm) and developed by the institute of petrochemical engineering, dalian, of the China petrochemical industry, inc.; the temperature of a hydrogenation reaction zone of the first boiling bed is 410 ℃, the reaction pressure is 12.0MPa, the hydrogen-oil ratio is 700, and the liquid hourly space velocity is 1.0 h -1 (ii) a The temperature of a hydrogenation reaction zone of the second boiling bed is 425 ℃, the reaction pressure is 12.0MPa, the hydrogen-oil ratio is 700, and the liquid hourly space velocity is 0.5 h -1 (ii) a The specific test results are shown in Table 2.
Comparative example 1
The main difference between the comparative example and the present invention is that the fractionation unit 9 is arranged behind the second ebullated-bed hydrogenation reaction zone, and the pretreated aromatic-rich component of the catalytic diesel directly enters the first ebullated-bed hydrogenation reaction zone. The main process flow of the comparative example is that the catalytic diesel oil 1 enters a pretreatment unit 2, contacts with a pretreatment agent 4 and is separated to obtain an aromatic hydrocarbon-rich component 6 and an alkane-rich component 5; the obtained aromatic hydrocarbon-rich component enters a pretreatment agent recovery unit 3, and is separated to obtain an aromatic hydrocarbon fraction 7 and a regeneration pretreatment agent 8, wherein the regeneration pretreatment agent 8 can be recycled to be used by the pretreatment unit; the obtained aromatic hydrocarbon fraction 7 and hydrogen 14 enter a first fluidized bed hydrogenation reaction zone 13, and hydrogenation reaction is carried out under the action of a first hydrogenation catalyst and hydrogen to generate a first reaction effluent 15; the obtained first reaction effluent 15 and hydrogen 14 enter a second boiling bed hydrogenation reaction zone 16, and react under the action of a second hydrogenation catalyst and hydrogen to generate a second reaction effluent 17, the second reaction effluent 17 enters a separation unit, the separation unit comprises a first high-pressure separator 18 and a low-pressure separator 19, gas 20 and a liquid phase 21 are obtained after separation by the high-pressure separator, the liquid phase 21 further enters the low-pressure separator 19 to obtain dry gas 22 and a liquid phase 23, and the obtained liquid phase 23 enters a fractionation unit 9 to be separated into a gas phase 24, a light fraction 10 and a heavy fraction 25.
The pretreatment unit is an aromatic hydrocarbon extraction device, the extracting agent is sulfolane, the extraction temperature is 170 ℃, and the mass ratio of the extracting agent to the oil is 15.0; and (3) introducing the extracted aromatic-rich component into a fractionation unit, wherein the dry point temperatures of the light fraction and the middle fraction are 220 ℃ and 310 ℃ respectively. The first boiling bed reaction zone and the second boiling bed reaction zone adopt the same hydrogenation catalyst, the hydrogenation catalyst adopts FC-70 catalyst which is subjected to fragmentation treatment (is crushed into short strips with the diameter of 0.5-1.0 mm) and developed by the institute of petrochemical engineering, dalian of the China petrochemical industry, inc., and the petrochemical industry research institute, wherein the hydrogenation catalyst adopted by the second boiling bed reaction zone is the catalyst after the first boiling bed reaction zone operates for 3 months; the temperature of a hydrogenation reaction zone of the first boiling bed is 405 ℃, the reaction pressure is 10.0MPa, the hydrogen-oil ratio is 800, and the liquid hourly volume space velocity is 1.2h -1 (ii) a The temperature of a hydrogenation reaction zone of the second fluidized bed is 420 ℃, the reaction pressure is 10.0MPa, the hydrogen-oil ratio is 800, and the liquid hourly space velocity is 0.6 h -1 (ii) a The specific test results are shown in the table2。
TABLE 2 hydrogen consumption and product (stream 10) hydrocarbon composition for catalytic diesel hydroconversion
Claims (24)
1. A catalytic diesel oil combined treatment process comprises the following steps:
(1) The catalytic diesel oil enters a pretreatment unit, contacts with a pretreatment agent and is separated to obtain an aromatic hydrocarbon-rich component and an alkane-rich component;
(2) Separating the aromatic hydrocarbon-rich component obtained in the step (1) to obtain aromatic hydrocarbon fraction and a regeneration pretreating agent;
(3) The aromatic hydrocarbon fraction obtained in the step (2) enters a fractionation unit, and a first gas phase, a light fraction, a middle fraction and a heavy fraction are obtained after separation;
(4) The heavy fraction obtained in the step (3) enters a first boiling bed hydrogenation reaction zone, and hydrogenation reaction is carried out under the action of a first hydrogenation catalyst and hydrogen to generate a first reaction effluent;
(5) Allowing the middle distillate obtained in the step (3) and the first reaction effluent obtained in the step (4) to enter a second fluidized bed hydrogenation reaction zone, reacting under the action of a second hydrogenation catalyst and hydrogen to generate a second reaction effluent, performing gas-liquid separation on the second reaction effluent to obtain a second gas phase and a second liquid phase, and allowing the obtained liquid phase to enter the fractionation unit in the step (3) for treatment;
the process conditions of the first boiling bed hydrogenation reaction zone are as follows: the reaction temperature is 350-450 ℃, the reaction pressure is 5.0-15.0 MPa, the volume ratio of hydrogen to oil is 500-2000, and the liquid hourly space velocity is 0.1-5.0 h -1 (ii) a The process conditions of the hydrogenation reaction zone of the second boiling bed are as follows: the reaction temperature is 350-450 ℃, the reaction pressure is 5.0-15.0 MPa, the volume ratio of hydrogen to oil is 500-2000, and the liquid hourly space velocity is 0.1-5.0 h -1 。
2. A catalytic diesel fuel combination treatment process according to claim 1, wherein in step (1) the catalytic diesel fuel has an aromatics content higher than 50wt%.
3. A catalytic diesel fuel combination treatment process according to claim 1 or 2, wherein the aromatic content in the catalytic diesel fuel in step (1) is 55wt% to 80wt%.
4. The catalytic diesel oil combined treatment process according to claim 1, wherein the pretreatment agent in the step (1) is at least one selected from sulfone compounds, aldehyde compounds, alkanone compounds, amide compounds and ionic liquids.
5. The catalytic diesel oil combined treatment process according to claim 1 or 4, wherein the pretreating agent in the step (1) is a sulfone compound.
6. The catalytic diesel combined treatment process according to claim 1 or 4, wherein the pretreating agent in the step (1) is sulfolane, N-methyl pyrrolidone, N-dimethyl acetamide, caprolactam, [ emim]N(CN) 2 、[3-mebupy]N(CN) 2 At least one of (a).
7. The catalytic diesel combination treatment process of claim 1, wherein the pretreatment unit operating conditions in step (1) are: the temperature is 30-200 ℃, and the mass ratio of the pretreating agent to the catalytic diesel oil is 0.5-25.0.
8. The catalytic diesel combination treatment process of claim 1, wherein the pretreatment unit operating conditions in step (1) are: the temperature is 30-180 ℃, and the mass ratio of the pretreating agent to the catalytic diesel oil is 5.0-20.0.
9. The process for the combined treatment of catalytic diesel oil according to claim 1, wherein the cutting temperature of the light fraction and the middle fraction in step (1) is 150-250 ℃ and the cutting temperature of the middle fraction and the heavy fraction is 260-320 ℃.
10. The process for the combined treatment of catalytic diesel fuel according to claim 1, wherein the cutting temperature of the light fraction and the middle fraction in step (1) is between 180 ℃ and 220 ℃ and the cutting temperature of the middle fraction and the heavy fraction is between 290 ℃ and 310 ℃.
11. The catalytic diesel oil combination treatment process according to claim 1, wherein the first hydrogenation catalyst and the second hydrogenation catalyst filled in the first ebullated bed hydrogenation reaction zone and the second ebullated bed hydrogenation reaction zone are the same or different.
12. The catalytic diesel combined treatment process according to claim 1, wherein the second hydrogenation catalyst used in the second ebullated-bed hydrogenation reaction zone is discharged to the first ebullated-bed hydrogenation reaction zone to be used as the first hydrogenation catalyst.
13. The catalytic diesel oil combination treatment process according to claim 1, wherein the alkane-rich component obtained in step (1) is returned to a catalytic cracking unit for treatment, or is used as a raw material for preparing olefin by a steam cracking unit and a catalytic cracking unit.
14. The catalytic diesel oil combination treatment process according to claim 1, wherein the process conditions of the first ebullated-bed hydrogenation reaction zone in the step (4) are as follows: the reaction temperature is 380-440 ℃, the reaction pressure is 8.0-18.0 MPa, the volume ratio of hydrogen to oil is 600-1500, and the liquid hourly space velocity is 0.2-2.0 h -1 。
15. The catalytic diesel combined treatment process according to claim 1, wherein the process conditions of the second ebullated-bed hydrogenation reaction zone in the step (5) are as follows: the reaction temperature is 380-440 ℃, the reaction pressure is 8.0-18.0 MPa, the volume ratio of hydrogen to oil is 600-1500, and the liquid hourly space velocity is 0.2-2.0 h -1 。
16. The catalytic diesel oil combination treatment process according to claim 1, wherein the reaction temperature of the second ebullated-bed hydrogenation reaction zone in the step (5) is 5-30 ℃ higher than that of the first ebullated-bed hydrogenation reaction zone in the step (4).
17. A catalytic diesel combination treatment process according to claim 1 or 16, wherein the reaction temperature of the second ebullated-bed hydrogenation reaction zone in step (5) is 5 to 15 ℃ higher than the reaction temperature of the first ebullated-bed hydrogenation reaction zone in step (4).
18. A catalytic diesel combined treatment system, the combined treatment system comprising:
the pretreatment unit is used for receiving and treating catalytic diesel and a pretreatment agent to obtain a component rich in alkane and a component rich in aromatic hydrocarbon after treatment;
the pretreatment agent recovery unit is used for receiving the aromatic hydrocarbon-rich component from the pretreatment unit, separating to obtain an aromatic hydrocarbon fraction and a regenerated pretreatment agent, and returning the regenerated pretreatment agent to the pretreatment unit for recycling;
the fractionation unit is used for receiving and processing the aromatic hydrocarbon fraction from the pretreatment agent recovery unit, and separating to obtain a light fraction, a middle fraction and a heavy fraction;
the first ebullated bed hydrogenation reaction zone is used for receiving the heavy fraction from the fractionation unit and reacting under the action of hydrogen and a first hydrogenation catalyst to obtain a first reaction effluent;
and the second boiling bed hydrogenation reaction zone is used for receiving the first reaction effluent from the first boiling bed hydrogenation reaction zone and the middle fraction from the fractionation unit, reacting under the action of hydrogen and the first hydrogenation catalyst to obtain a second reaction effluent, treating the second reaction effluent in the separation unit, and treating the liquid phase obtained after separation in the fractionation unit.
19. The catalytic diesel combined treatment system of claim 18, wherein the pretreatment unit employs a solvent refining unit or an aromatics extraction unit.
20. The catalytic diesel combined treatment system of claim 18, wherein the first ebullated-bed hydrogenation reaction zone is provided with more than one ebullated-bed reactor.
21. The catalytic diesel combined treatment system of claim 20, wherein an ebullated-bed reactor with a three-phase separator disposed therein is used.
22. The catalytic diesel combined treatment system of claim 18, wherein the second ebullated-bed hydrogenation reaction zone is provided with more than one ebullated-bed reactor.
23. The catalytic diesel combined treatment system of claim 22, wherein an ebullated-bed reactor with a three-phase separator disposed therein is used.
24. The catalytic diesel combined treatment system of claim 18, wherein the separation unit comprises a gas-liquid separator and a fractionation column.
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| CN102443436A (en) * | 2010-10-12 | 2012-05-09 | 中国石油化工股份有限公司 | Combined method for hydrotreatment, catalytic cracking and diesel oil aromatic extraction of residual oil |
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