WO2012142723A1 - Procédé combiné pour l'hydrogénation et le craquage catalytique de pétrole résiduaire - Google Patents

Procédé combiné pour l'hydrogénation et le craquage catalytique de pétrole résiduaire Download PDF

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Publication number
WO2012142723A1
WO2012142723A1 PCT/CN2011/000683 CN2011000683W WO2012142723A1 WO 2012142723 A1 WO2012142723 A1 WO 2012142723A1 CN 2011000683 W CN2011000683 W CN 2011000683W WO 2012142723 A1 WO2012142723 A1 WO 2012142723A1
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Prior art keywords
catalytic cracking
residue
hydrogenation
oil
hydrotreating
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PCT/CN2011/000683
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English (en)
Chinese (zh)
Inventor
关明华
刘铁斌
耿新国
张学萍
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中国石油化工股份有限公司
中国石油化工股份有限公司抚顺石油化工研究院
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Priority to PCT/CN2011/000683 priority Critical patent/WO2012142723A1/fr
Publication of WO2012142723A1 publication Critical patent/WO2012142723A1/fr

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Classifications

    • 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
    • C10G69/02—Treatment of hydrocarbon oils by at least one hydrotreatment process and at least one other conversion process plural serial stages only
    • C10G69/04—Treatment of hydrocarbon oils by at least one hydrotreatment process and at least one other conversion process plural serial stages only including at least one step of catalytic cracking in the absence of hydrogen
    • 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
    • C10G2300/42—Hydrogen of special source or of special composition
    • 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
    • C10G2400/00—Products obtained by processes covered by groups C10G9/00 - C10G69/14
    • C10G2400/02—Gasoline

Definitions

  • the invention relates to a method for purifying a residue, in particular to a method for organically combining residue hydrotreating and catalytic cracking, and mainly producing gasoline products using residual oil as a raw material.
  • the processing of heavy and residual oil is not only to crack it into low-boiling products, such as naphtha, intermediate oil and vacuum gas oil, but also to increase their hydrogen-to-carbon ratio. Carbon or hydrogenation methods are used to achieve this.
  • the decarburization process includes coking, solvent deasphalting, heavy oil catalytic cracking, etc.; hydrogenation includes hydrocracking, hydrorefining, and the like.
  • the hydrogenation process can hydrogenate the residue to improve the yield of the liquid product, and can also remove the hetero atoms therein, and the product quality is good.
  • the hydrogenation process is a catalytic process, and there is a problem of deactivation of the hydrogenation catalyst.
  • the residual oil cracking rate of the residue hydrotreating technology is low, and the main purpose is to provide raw materials for downstream raw material lightening equipment such as catalytic cracking or coking.
  • the content of impurities such as sulfur, nitrogen, metal and the residual carbon in the inferior residue are significantly reduced, thereby obtaining a feed acceptable to the downstream lightening device, especially the catalytic cracking device, so the current heavy and slag
  • the combined technology of residual oil hydrotreating and catalytic cracking of residual oil is the mainstream technology.
  • the existing residue hydrotreating and catalytic cracking combined process firstly hydrotreats the residue, hydrolyzes the oil to separate the naphtha and the diesel fraction, and the hydrogenated tail oil acts as a heavy oil catalytic cracking feed for catalytic cracking.
  • the reaction is a dry gas, a liquefied gas, a gasoline, a diesel oil and a coke, a reductive oil is subjected to catalytic refining or a recirculating oil refining device is mixed with a residue hydrotreating raw material for hydrotreating, and the catalytic oil slurry is externally or partially Catalytic refining or recycling back to residual oil Hydrogenation unit.
  • the combination process of the above-mentioned residue hydrotreating and catalytic cracking has disadvantages such as low gasoline yield, large heat energy loss, and high equipment investment.
  • No. 4,713,221 discloses the recycling of catalytically cracked heavy cycle oil to a residue hydrotreating unit on the basis of a combination of conventional residue hydrogenation and catalytic cracking, mixing with the residue, hydrogenation, and then entering the catalytic cracking unit.
  • the catalytic cracking slurry has not been effectively utilized, and the method has a limited yield for reducing coke yield and increasing product yield.
  • CN1119397C discloses a residue hydrotreating-catalytic cracking combined process, in which a residue and a clarified oil are fed together into a residue hydrogenation unit, and reacted in the presence of hydrogen and a hydrogenation catalyst, and the heavy cycle oil is catalyzed.
  • the inside of the cracking unit is circulated; the oil slurry obtained by the reaction is separated by a separator to obtain a clarified oil, and is returned to the hydrogenation unit.
  • the slurry enters the residue hydrotreating unit, and the cokes in the slurry will increase the carbon deposition of the hydrogenation catalyst, reduce the hydrogenation activity and operation cycle of the hydrogenation catalyst, and the heavy cycle oil is in the catalytic cracking. Inside the device. Therefore, this method is limited in reducing coke yield and improving product quality.
  • CN1382776A discloses a combined method of residue hydrotreating and heavy oil catalytic cracking, which comprises hydrogenating a residue in a hydrotreating unit, separating the reaction product to obtain a gas, hydrogenating naphtha, hydrogenated diesel and adding Hydrogen residue.
  • the resulting hydrocracked oil enters a catalytic cracking unit for cracking reaction together with an optional vacuum gas oil, and the catalytically cracked heavy cycle oil is returned to the hydrotreating unit, and the distillate obtained by distilling the slurry is returned to the hydrotreating unit.
  • the method organically combines two units to convert residual oil, heavy cycle oil and slurry into light oil.
  • the method has a fractionation system in both the hydrotreating and the catalytic cracking process, which increases the investment cost; the heat energy loss is more due to the process heat exchange; meanwhile, the hydrotreating device and the catalytic cracking device have diesel products, relatively speaking, , the total yield of gasoline and gas products will be reduced.
  • the residual oil cracking rate of the residue hydrotreating unit is low, and the yield of naphtha and diesel oil obtained by fractionating the hydrogenated oil is limited, and the diesel fraction obtained by the hydrotreating process of the residue still cannot satisfy the high quality.
  • Catalytic cracking diesel sulfur and other impurities are high in content and poor in nature, and further hydrotreating is required to be a qualified diesel product.
  • the present invention provides a residue hydrotreating and catalytic cracking
  • the combined method can produce gasoline products in the largest amount, and the process is simple and the overall energy consumption is reduced.
  • the combination method of the residue hydrotreating and catalytic cracking of the present invention comprises: the residue raw material is subjected to hydrogenation reaction in the presence of hydrogen and a hydrotreating catalyst, and the hydrogenation reaction effluent is gas-liquid separated to obtain a gas phase and a liquid phase, and the gas phase cycle is used for In the hydrogenation reaction, the liquid phase directly enters the catalytic cracking unit without fractionation, and the catalytic cracking heavy fraction after the catalytic cracking reaction effluent separates the dry gas, the liquefied gas and the catalytic cracked gasoline is mixed with the residue raw material for hydrogenation reaction.
  • the residue raw material comprises atmospheric residue or vacuum residue, and may also be a residue raw material of other sources, and the residue raw material may also contain partial coking wax oil, deasphalted oil, heavy distillate oil.
  • the hydrogenation reaction effluent is first subjected to gas-liquid separation, and the gas-liquid separation is carried out under the same conditions as the reaction pressure level to obtain a gas phase and a liquid phase, the gas phase is mainly hydrogen gas, and is subjected to selective dehydrogenation treatment and then recycled.
  • the hydrogenation reaction process needs to be supplemented with new hydrogen to supplement the consumption of the reaction process.
  • the pressure separator controls the pressure of the low pressure separator at the pressure of the catalytic cracking unit and then directly enters the catalytic cracking unit, and the equipment such as the feed pump of the catalytic cracking unit can be eliminated.
  • the low pressure separator can flash a small amount of light hydrocarbons and dissolve. Hydrogen sulfide, hydrogen, etc.
  • the gas-liquid separation of the present invention employs conventional separation means, and includes, for example, the use of a conventional gas-liquid separation tank, a hydrocyclone, and the like. However, it does not include a fractionation unit, which greatly reduces equipment investment and reduces energy consumption.
  • the residue hydrogenation technology can be any technology suitable for the present invention, such as fixed bed residue hydrotreating technology, suspended bed residue hydrotreating technology, fluidized bed residue hydrotreating technology, moving bed residue hydrotreating Technology, etc.
  • the residual hydrotreating catalyst used has the functions of hydrodemetallization, hydrodesulfurization, hydrodenitrogenation and hydrocracking of residual oil. Single catalyst or combined catalyst. These catalysts are generally supported by a porous refractory inorganic oxide such as alumina, and an oxide of Group VIB and/or Group VIII metals such as W, Mo, Co, Ni, etc. as an active component, optionally added to each other.
  • the sulfur catalyst and the hydrodenitrogenation catalyst are generally loaded in such a manner that the feedstock oil is sequentially contacted with a protective agent, a hydrodemetallization, a hydrodesulfurization, and a hydrodenitrogenation catalyst.
  • a protective agent e.g., a hydrodemetallization, a hydrodesulfurization, and a hydrodenitrogenation catalyst.
  • Hydrotreating generally requires multiple reactors to increase throughput. It is usually operated at an absolute pressure of from about 5 MPa to about 35 MPa, preferably from about 10 MPa to about 20 MPa, at a temperature of from about 300 ° C to about 500 ° C, preferably from about 350 ° C to about 450 ° C.
  • the liquid hour volumetric space velocity and hydrogen partial pressure are selected according to the characteristics of the material to be treated and the required conversion rate and depth of refining.
  • the volumetric space velocity of the fresh residue raw material liquid is generally in the range of about 0.1 h - about 5.01 T 1 , preferably about 0.15 h - about S. Oh, and the total hydrogen oil volume ratio is from about 100 to about 5,000, preferably About 300 - about 3000.
  • the invention is suitable for hydrocracking of atmospheric and vacuum residue, and is especially suitable for hydroconversion of heavy hydrocarbon oil.
  • the specific conditions of the residue hydrotreating process can be specifically determined based on the nature of the feedstock and the requirements of the feed to the catalytic cracking unit.
  • catalytic cracking can employ conventional techniques in the art.
  • the catalytic cracking unit may be one or more than one set, and each unit shall include at least one reactor and one regenerator.
  • the catalytic cracking reaction effluent can be separated into dry gas, liquefied gas, catalytically cracked gasoline, and catalytically cracked heavy ends using conventional techniques in the art.
  • the catalytic cracking unit may be provided with a fractionator, which may be set separately or shared for each set of catalytic cracking units.
  • the catalytic cracking fractionation column fractionates the catalytic cracking reaction effluent into dry gas, liquefied gas, catalytically cracked gasoline, and catalytically cracked heavy ends.
  • the catalytic cracking fractionation column used in the present invention can be simply designed in comparison with a conventional catalytic cracking fractionation tower, and only fractionated dry gas, liquefied gas and catalytically cracked gasoline, and the catalytic cracking heavy fraction is divided into an initial boiling point of 170 - 220 °C.
  • the fractions include catalytic cracking diesel, catalytic cracking heavy cycle oil and slurry.
  • the catalytic cracking heavy fraction is filtered to remove the trace catalytic cracking catalyst powder before being recycled to the hydrotreating unit.
  • the catalytic cracking unit is operated under the general conditions of the art: a reaction temperature of from about 450 to about 600 ° C, preferably from about 480 to about 550 ° C; a regeneration temperature of from about 600 to about 800 ° C, preferably from about 650 to about At 750 ° C, the weight ratio of the extender oil is from about 2 to about 30, preferably from about 4 to about 10; the contact time with the catalyst is from about 0.1 to about 15 seconds, preferably from about 0.5 to about 5 seconds; and the pressure is about 0.1. ⁇ about 0.5MPa.
  • the catalytic cracking catalysts used include catalysts commonly used for catalytic cracking, such as silica-alumina catalysts, silico-magnesium catalysts, acid-treated clays, and molecular sieve cracking catalysts such as X-type, Y-type, ZSM-5, M-type, and pillar columns. It is a molecularly cleavable catalyst', because the molecular cleavage catalyst has high activity, less coke formation, high gasoline yield and high conversion rate.
  • Catalytic cracking unit The reactor may be of various types of catalytic cracking reactors, preferably riser reactors or riser extra bed reactors.
  • the process flow is generally as follows:
  • the feedstock oil is injected from the bottom of the riser reactor, and is contacted with a high-temperature regenerated catalyst from the regenerator, and the catalyst mixture formed by the cracking reaction and the coke-deposited catalyst moves upward along the riser reactor to complete the catalysis of the whole feedstock oil.
  • Cracking reaction Material ⁇ and production ⁇ .
  • Quality indicators are obtained through simple experiments. P , , , and the advantages of the present invention are:
  • the hydrotreating unit does not have a fractionation system
  • the hydrogenated oil directly enters the catalytic cracking reactor, and the catalytic cracking produces oil.
  • the remaining mixed oil is filtered and recycled to the hydrogenation unit. Both processes greatly reduce heat loss and achieve hot feed, which reduces energy consumption throughout the process.
  • the main products are high-octane catalytic cracking gasoline, liquefied petroleum gas and a small amount of dry gas, so as to ensure the maximum production of gasoline.
  • the gasoline obtained by the present invention has a high octane number and a marked improvement in quality.
  • the catalytic cracking of diesel fuel obtained by the prior scheme has a high content of aromatic hydrocarbons, a low cetane number, a high content of impurities such as sulfur, and poor properties, and further hydrotreating is required as a qualified diesel product.
  • the separation system of the catalytic cracking reaction effluent of the present invention does not carry out the separation of the catalytically cracked diesel fraction, eliminating the need for repeated processing steps.
  • the catalytic cracking fractionation column of the present invention can be greatly simplified, reducing equipment investment and operating energy consumption.
  • the catalytic cracking reaction effluent does not separate the catalytic cracking oil slurry, and solves the problem that the oil slurry is difficult to separate the catalyst solid powder due to the large viscosity.
  • the catalytic cracking heavy distillate contains a diesel fraction. Due to the dilution effect of the diesel split, the viscosity of the catalytic cracking slurry is greatly reduced, making the catalyst solid powder filtration easier.
  • the utilization rate is low, and the method of the invention does not separate the catalytic cracking slurry, and does not generate an efflux portion, thereby improving the utilization rate of the raw materials and the intended production. The yield of the product.
  • the catalytic cracking heavy fraction dilutes the fresh residue raw material, improves the oil properties, reduces the difficulty of hydrogenation reaction and the processing severity of the residue hydrotreating mixed feed; in addition, the catalytic cracking heavy fraction can be reduced
  • the viscosity of the raw materials improve the distribution of the raw materials in the reaction system and the transmission shield, reduce the influence of diffusion in the hydrotreating process of the residue, improve the deposition distribution of harmful metals such as nickel and vanadium in the catalytic reaction system, and prolong the catalyst. Service life; At the same time, the reduction in viscosity makes it easier to transport and filter the mixed feedstock.
  • the catalytic cracking diesel oil fraction and the above heavy fraction can remove impurities during the residue hydrogenation process, and the aromatic hydrocarbons are saturated, which becomes a better catalyzed, chemically cracked raw material composition, further improving the yield of high value-added products of catalytic cracking, The low value coke yield is significantly reduced.
  • FIG. 1 is a schematic view showing the process flow of a combined method of residue hydrotreating and catalytic cracking according to the present invention. detailed description
  • the residue raw material 1 and the filtered catalytically cracked heavy fraction 17 are mixed, and after being pressurized, mixed with the circulating hydrogen 2 to enter the hydrotreating reactor 3, and the metal and sulfur in the raw material oil are removed by contact with the hydrotreating catalyst bed. Impurities such as nitrogen, while reducing the residual carbon of the raw materials to meet the feed requirements of the downstream catalytic cracking unit.
  • Hydrogenation reactor 3 The outlet reaction effluent 4 enters the high pressure separator 5 for gas-liquid separation, and the separated gas phase stream is subjected to dehydrogenation treatment or the like, and then the compressor 8 is pressurized and recycled to the inlet of the hydrotreating reactor 3.
  • the supplemented new hydrogen can also be introduced after the recycle compressor 8, and the separated liquid phase stream is further separated into the helium separator 6, and the separated liquid phase stream is not subjected to heat exchange and fractionation to adjust the pressure of the low pressure separator.
  • the liquid phase stream is passed through line 7 to reaction system 9 of the catalytic cracking unit without the use of a feed pump.
  • the hydrogenated oil from line 7 enters the reaction system 9 of the catalytic cracking unit, contacts and reacts with the high temperature regenerated catalytic cracking catalyst, and the reacted oil and gas stream 10 enters the fractionation column 13 of the catalytic unit to separate the gas 11 and catalytic cracking.
  • Gasoline 12, gas 11 and catalytic cracking gasoline 12 discharge device, and the remaining catalytic cracking heavy fraction 14 of the fractionation column enters the separator 15.
  • the catalyst powder, impurities and solid particles 16 are filtered off, and the filtered catalytically cracked heavy fraction 17 is recycled to the hydrotreating unit.
  • the reaction is carried out on a small riser tubular catalytic cracking unit and a pilot residue oil hydrotreating unit.
  • the feedstock oil used in the examples and comparative examples was a normal crude oil of Saudi medium crude oil, the properties of which are shown in Table 1.
  • the type and volume of the residue hydrotreating catalyst used in the examples and the comparative examples are identical, and both are CEN, FZC, ZTN, ZTS series residue hydrogenation catalysts produced by the Catalyst Branch of China Petroleum & Chemical Corporation, including Protecting agent, demetallization catalyst, desulfurization catalyst, denitrification catalyst, etc., the filling sequence is generally to make the raw material oil in contact with the protective agent, hydrodemetallization, hydrodesulfurization, hydrodenitrogenation catalyst, of course, there are also these catalysts Hybrid loading technology.
  • the above catalyst loading technique is well known to those skilled in the art.
  • the catalytic cracking catalysts used in the examples and the comparative examples were the same as those used in the Dalian Petrochemical Company's 3.5 million tons/year heavy oil catalytic cracking unit, and were industrial equilibrium catalysts.
  • the composition of the freshener is: 95wt% LBO-16 hydroquinone catalyst + 5wt% LBO-A to increase the octane auxiliary.
  • This comparative example employs a conventional residue hydrotreating-catalytic cracking method in which a residue is subjected to a hydrogenation reaction in a hydrogenation treatment apparatus to separate a reaction product to obtain a gas, a hydrogenated naphtha, a hydrogenated diesel oil, and a hydrogenated residue.
  • the obtained hydrocracking oil enters a catalytic cracking unit for cracking reaction, and the catalytic cracking heavy-cycle oil is circulated in the catalytic cracking unit.
  • Table 2, Table 3 and Table 4 are the process conditions, product distribution and main product properties.
  • This embodiment adopts the combination method of residue hydrotreating and catalytic cracking provided by the invention, and all the liquid phase products of the hydrotreating process are directly into the catalytic cracking unit without fractionation, and the catalytic cracking reaction effluent fractionation system is simplified, and only the dry gas is fractionated.
  • the liquefied gas and the gasoline fraction, and the remaining catalytically cracked heavy fractions are filtered to the solid impurities and recycled to the hydrotreating unit for further processing.
  • Table 2, Table 3, and Table 5 are the process conditions, product distribution, and main product properties.

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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

L'invention porte sur un procédé combiné pour l'hydrogénation et le craquage catalytique de pétrole résiduaire. Dans le procédé, l'hydrogénation d'une matière première de type pétrole résiduaire est effectuée en présence d'hydrogène et d'un catalyseur d'hydrogénation; l'effluent de l'hydrogénation est soumis à une séparation gaz-liquide pour obtenir une phase gazeuse et une phase liquide; la phase gazeuse est utilisée en boucle pour l'hydrogénation; la phase liquide est directement introduite dans un dispositif de craquage catalytique sans fractionnement; après que les gaz secs, les gaz liquéfiés et le produit de craquage catalytique d'essence sont séparés de l'effluent de la réaction de craquage catalytique, la fraction lourde du craquage catalytique est obtenue et mélangée avec une matière première d'hydrogénation pour subir une hydrogénation. Par comparaison avec l'état de la technique, le procédé permet de produire de l'essence avec un rendement de production maximal et permet de faire des économies sur les coûts d'investissement en matériel, d'utiliser totalement l'énergie thermique de la réaction et de réduire la consommation d'énergie pour la production en même temps.
PCT/CN2011/000683 2011-04-19 2011-04-19 Procédé combiné pour l'hydrogénation et le craquage catalytique de pétrole résiduaire WO2012142723A1 (fr)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US11891578B2 (en) 2018-07-16 2024-02-06 China Petroleum & Chemical Corporation Process and system for catalytic cracking of hydrocarbon oils

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4713221A (en) * 1984-05-25 1987-12-15 Phillips Petroleum Company Crude oil refining apparatus
CN1262306A (zh) * 1999-01-28 2000-08-09 中国石油化工集团公司 一种渣油加氢处理－催化裂化组合工艺方法
CN101875855A (zh) * 2009-04-30 2010-11-03 中国石油化工股份有限公司 一种渣油加氢处理和催化裂化组合方法

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4713221A (en) * 1984-05-25 1987-12-15 Phillips Petroleum Company Crude oil refining apparatus
CN1262306A (zh) * 1999-01-28 2000-08-09 中国石油化工集团公司 一种渣油加氢处理－催化裂化组合工艺方法
CN101875855A (zh) * 2009-04-30 2010-11-03 中国石油化工股份有限公司 一种渣油加氢处理和催化裂化组合方法

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US11891578B2 (en) 2018-07-16 2024-02-06 China Petroleum & Chemical Corporation Process and system for catalytic cracking of hydrocarbon oils

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