CN115926839A - Catalytic cracking method for producing low-carbon olefin by Fischer-Tropsch synthetic oil - Google Patents
Catalytic cracking method for producing low-carbon olefin by Fischer-Tropsch synthetic oil Download PDFInfo
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- 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
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/584—Recycling of catalysts
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Abstract
The invention discloses a catalytic cracking method for producing low-carbon olefin by Fischer-Tropsch synthetic oil, which comprises the following steps: the Fischer-Tropsch synthesis oil enters a riser reactor and is subjected to contact reaction with a catalytic cracking regenerated catalyst to obtain a first reaction material flow, and the aromatic hydrocarbon raffinate oil is input into the riser reactor and is subjected to contact reaction with the first reaction material flow to obtain a second reaction material flow; the heavy oil enters the riser reactor above the aromatics raffinate oil feed inlet and contacts and reacts with the second reactant flow to obtain a third reactant flow; the carbon deposition catalyst enters a regenerator for regeneration through steam stripping of a stripping reactor, and the obtained regenerated catalyst enters a riser for cyclic reaction; and the mixed oil steam obtained after the steam stripping of the third reactant flow enters a condenser to obtain gas-phase and liquid-phase products. The method improves the yield of the low-carbon olefin under the condition of not reducing the octane number of the gasoline, and reduces the yield of the coke by 3 percent on the premise of meeting the thermal balance of the device.
Description
Technical Field
The invention discloses a processing method under the synergistic action of Fischer-Tropsch synthetic oil and aromatic raffinate oil, and particularly relates to a method for producing low-carbon olefins by carrying out catalytic cracking reaction on Fischer-Tropsch synthetic oil and aromatic raffinate oil.
Background
With the increasing consumption of petroleum resources and the enhancement of environmental awareness of people, the synthesis of liquid fuel from coal and natural gas has become an important way to replace petroleum energy. The fluid catalytic cracking process is a core process in oil refinery technology not only because it is a major means of heavy oil processing, a major source of light oil components, but also has an irreplaceable position in providing light olefins and petrochemical integrated technologies. The Fischer-Tropsch synthesis product has higher purity, does not contain other impurities basically, is saturated normal hydrocarbon basically, and has less content of isomeric hydrocarbon and olefin, so the Fischer-Tropsch synthesis light oil has lower octane number and is not suitable for being used as motor gasoline; the Fischer-Tropsch synthetic heavy oil has high cetane number, but has poor low-temperature fluidity and higher condensation point. The aromatic raffinate oil is the remaining low-carbon alkane substance after the C6 and C7 components in the catalytic cracking and reforming product oil are subjected to aromatic extraction; at present, raffinate oil is mainly used for producing solvent oil, the utilization of added value is not basically improved, and part of raffinate oil is returned to a cracking furnace to be used as cracking raw material, but the olefin yield in the cracking process is low due to high content of cycloparaffin. Therefore, both Fischer-Tropsch synthetic oil and aromatic raffinate oil need to be processed for the second time so as to widen the application range and improve the economic benefit.
Chinese patent CN 102533322B discloses a method for producing propylene by catalytic cracking Fischer-Tropsch synthetic oil, which mixes material flow rich in micromolecular olefin (C4-C5) with Fischer-Tropsch synthetic oil raw material and injects the mixture into a reactor. Not only can process heavy Fischer-Tropsch synthetic oil fractions, but also can process light Fischer-Tropsch synthetic oil fractions. Under the same reaction conditions, the yield of the propylene is improved by 6.74 percentage points; but the coke yield is too low to satisfy the heat balance of the self-reaction-regeneration system.
Chinese patent CN 106609151B discloses a method for producing low-carbon olefins, which comprises the steps of carrying out a first catalytic cracking reaction on conventional petroleum and a catalytic cracking catalyst, and then carrying out a second catalytic cracking reaction on a reaction mixture obtained by the first catalytic cracking reaction and Fischer-Tropsch synthetic oil, so that the conversion of the Fischer-Tropsch synthetic oil and the conventional petroleum can be promoted, the selectivity of the low-carbon olefins is improved, and the highest yield of trienes (ethylene, propylene and butylene) is 42.95 wt%. The method does not describe the change of the octane value of the gasoline.
Chinese patent CN 105567307B discloses a method for producing low-carbon olefin from Fischer-Tropsch synthetic oil, which comprises the steps of carrying out thermal cracking reaction on the Fischer-Tropsch synthetic oil, and then contacting the obtained reactant flow with a catalytic cracking catalyst to carry out catalytic cracking reaction, so that the yield of the low-carbon olefin (ethylene + propylene + butylene) is obviously improved by 49.45 wt%. However, the reaction process of the method needs to pass through a fixed bed reactor and a fluidized bed reactor, the process is complex, and the change situation of the gasoline octane value is not explained.
Chinese patent CN101362959B discloses a catalytic conversion method for preparing propylene and high-octane gasoline, in which the raw material difficult to crack is firstly contacted with a thermal regeneration catalyst, and the temperature is 600-750 ℃, the weight hourly space velocity is 100-800h －1 Pressure of 0.10-1.0MPa, catalyst and raw materialThe weight ratio of 30-150, the weight ratio of water vapor and raw material is 0.05-1.0, the cracking reaction is carried out, the reactant flow is mixed with the raw oil which is easy to crack, the temperature is 450-620 ℃, the weight hourly space velocity is 0.1-100h －1 The pressure is 0.10-1.0MPa, the weight ratio of the catalyst to the raw material is 1.0-30, and the weight ratio of the steam to the raw material is 0.05-1.0; after the spent catalyst and the reaction oil gas are separated, the spent catalyst enters a stripper, is stripped, burnt and regenerated and then returns to the reactor, the reaction oil gas is separated to obtain a target product propylene, high-octane gasoline and a recracked raw material, and the recracked raw material comprises a fraction with the distillation range of 180-260 ℃ and heavy aromatic raffinate oil. The yield of propylene in the method is 29.02 percent at most. However, the coke yield of this process is high (> 7%).
Chinese patent CN 105505463A discloses a heavy oil catalytic cracking method and apparatus, the reactor adopted in the method includes a first riser and a second riser, and the method includes contacting heavy oil raw material with a catalytic cracking catalyst in the first riser and making the heavy oil raw material and the catalytic cracking catalyst go upward to generate a first catalytic cracking reaction; fractionating the reaction oil gas to obtain cracked gas, gasoline, diesel oil, recycle oil and oil slurry; an aromatic hydrocarbon extraction solvent is used for carrying out dearomatization treatment on the recycle oil to obtain aromatic hydrocarbon extract oil and aromatic hydrocarbon raffinate oil; the aromatic hydrocarbon extract oil is subjected to catalytic hydrogenation reaction at the reaction temperature of 340-380 ℃ and the volume space velocity of 0.5-2.0h -1 The volume ratio of hydrogen to oil is 300-800, the reaction pressure is 7-12MPa, and the generated oil gas is fractionated to obtain cracked gas, gasoline, diesel oil and catalytic hydrogenation heavy oil; and introducing the catalytic hydrogenation heavy oil and the aromatic raffinate oil into a second riser to perform a second catalytic cracking reaction, and fractionating the reaction oil gas to obtain cracked gas, gasoline and diesel oil. The method and the device can realize the maximum production of light oil products and chemical raw materials with high added values, and simultaneously improve the utilization rate of heavy oil raw materials. However, the method does not particularly describe the yield of the low-carbon olefin and the RON of the gasoline, and the method has high energy consumption through a hydro-upgrading process, adopts two riser reactors and has a complex reaction process.
Chinese patent CN 101531558B discloses a catalytic conversion method for preparing propylene and aromatic hydrocarbon with different cracking performancesThe hydrocarbon raw material is contacted with a catalytic cracking catalyst at the temperature of 450-750 ℃ and the weight hourly space velocity of 0.1-800h -1 The method comprises the steps of performing cracking reaction in a fluidized bed reactor under the conditions that the reaction pressure is 0.10-1.0MPa, the weight ratio of a catalytic cracking catalyst to a raw material is 1-150, and the weight ratio of water vapor to the raw material is 0.05-1.0, separating spent catalyst and reaction oil gas, returning the spent catalyst to the reactor after regeneration, separating the reaction oil gas, and separating to obtain target products of low-carbon olefin, aromatic hydrocarbon and a recracked raw material, wherein the recracked raw material is subjected to hydrogenation treatment and then is recracked. The method produces the low-carbon olefins such as propylene and the like from the heavy raw materials to the maximum extent, wherein the yield of the propylene is more than 40 weight percent, and simultaneously produces the aromatic hydrocarbons such as toluene, xylene and the like, and the reduction range of the yield of dry gas is as high as more than 80 weight percent. However, in the method, the heavy oil raw material and the light aromatic raffinate oil which are re-cracked are subjected to a hydrotreating unit, so that the hydrogen consumption is increased, ethylene and butylene in the product are subjected to metathesis reaction to generate propylene, the whole method has a long flow, and the involved reaction process is complicated.
Chinese patent CN101362963A discloses a catalytic conversion method for producing more propylene and preparing aromatic hydrocarbon at the same time, hydrocarbon raw materials with different cracking performances are contacted with a catalytic cracking catalyst, the temperature is 450-750 ℃, and the weight hourly space velocity is 0.1-800h －1 The method comprises the steps of performing cracking reaction in a fluidized bed reactor under the conditions that the reaction pressure is 0.10-1.0MPa, the weight ratio of a catalytic cracking catalyst to a raw material is 1-150, and the weight ratio of water vapor to the raw material is 0.05-1.0, separating spent catalyst and reaction oil gas, returning the spent catalyst to the reactor after regeneration, and separating the reaction oil gas to obtain target products of low-carbon olefin and aromatic hydrocarbon and a recracked raw material. The method produces the low-carbon olefins such as propylene and the like from the heavy raw materials to the maximum extent, wherein the yield of the propylene is more than 40 weight percent, and meanwhile, the method produces the aromatics such as toluene, xylene and the like in a co-production way, and the reduction range of the yield of dry gas reaches more than 80 weight percent. However, in the method, the light aromatic raffinate oil which is re-cracked is subjected to a hydrotreating unit, so that the hydrogen consumption is increased, the heavy oil raw material which is re-cracked is subjected to an aromatic extraction process, ethylene and butylene in the product are subjected to metathesis reaction to generate propylene, the whole method has a long flow, and the involved reaction process is complicated.
Disclosure of Invention
In order to solve the defects of the prior art, the invention provides the catalytic cracking method for producing the low-carbon olefin from the Fischer-Tropsch synthetic oil, which can produce the low-carbon olefin under the synergistic effect of the Fischer-Tropsch synthetic oil and the aromatic raffinate oil, and can reduce the coke yield on the premise of keeping the octane number of gasoline not reduced and meeting the heat balance of a device. In addition, the catalytic cracking method for producing the low-carbon olefin by the Fischer-Tropsch synthetic oil does not need a hydrogenation process, and has the characteristics of low investment, short flow and quick response.
In order to achieve the above object, the present invention provides a catalytic cracking method for producing low carbon olefins from fischer-tropsch synthesis oil, comprising the following steps:
step (1): inputting Fischer-Tropsch synthetic oil into a riser reactor, and carrying out contact reaction on the Fischer-Tropsch synthetic oil and a catalytic cracking regenerated catalyst at an expanding section of the riser reactor to obtain a first reaction material flow;
step (2): inputting aromatic hydrocarbon raffinate oil into a riser reactor from the top of an expanding section, and carrying out contact reaction with a first reactant flow to obtain a second reactant flow;
and (3): inputting heavy oil into the riser reactor above the aromatics raffinate oil inlet, and allowing the heavy oil to contact and react with the second reactant flow to obtain a third reactant flow;
and (4): stripping the carbon deposition catalyst in the third reaction material flow through a stripping reactor, then entering a to-be-regenerated inclined tube through a settler, entering a regenerator for regeneration, and entering an obtained regenerated catalyst into a riser reactor for cyclic reaction; and the mixed oil steam obtained after the steam stripping of the third reactant flow enters a condenser to obtain a gas-phase product and a liquid-phase product.
The Fischer-Tropsch synthetic oil is hydrocarbons of C10-C34 in Fischer-Tropsch synthetic products.
The riser reactor is provided with a pre-lifting section and an expanding section in sequence from bottom to top along the vertical direction, and the lifting expanding section is positioned above a catalyst inlet.
The ratio of the diameter of the expanding section to the diameter of the pre-lifting section is 1.2-2.0.
The ratio of the length of the expanding section to the total length of the riser reactor is 0.05-0.10.
The aromatic raffinate oil of the invention is petroleum hydrocarbon fraction with the temperature of 70-150 ℃, and the quality content of naphthenic hydrocarbon of the aromatic raffinate oil is not less than 50%.
The heavy oil is slurry oil produced by a catalytic cracking process, and is at least one of heavy fraction and straight-run vacuum fraction generated by coking, thermal cracking and visbreaking processes.
The micro-reverse activity of the regenerated catalyst is 55-75%.
The Fischer-Tropsch synthetic oil accounts for 5 to 40 percent of the heavy oil by mass.
The mass ratio of the aromatic raffinate oil in the heavy oil is 10-40%.
The Fischer-Tropsch synthetic oil and the aromatic raffinate oil have the same or different dosages.
The outlet temperature of the riser reactor of the invention is 540-610 ℃.
The mass ratio of the regenerated catalyst to the heavy oil is 5-45.
The invention can also be detailed as follows:
the catalytic cracking method for producing the low-carbon olefin by the Fischer-Tropsch synthetic oil comprises the following steps: the Fischer-Tropsch synthetic oil enters a riser reactor from a Fischer-Tropsch synthetic oil feeding hole (1), and is subjected to contact reaction with a catalytic cracking regenerated catalyst in an expanding section of the riser reactor to obtain a first reaction material flow, and the aromatic raffinate oil enters the riser reactor from an aromatic raffinate oil feeding hole (2) (above the expanding section of the riser) and is subjected to contact reaction with the first reaction material flow to obtain a second reaction material flow; the heavy oil enters the riser reactor at a heavy oil feed inlet (3) above the aromatic raffinate oil feed inlet, and contacts and reacts with the second reactant flow to obtain a third reactant flow; the carbon deposition catalyst is stripped by a stripping reactor (7), then enters a spent inclined tube (8) through a settler (6), the spent catalyst enters a regenerator (10) for regeneration, and the obtained regenerated catalyst enters a riser reactor through a regeneration inclined tube (9) for cyclic reaction; and the mixed oil vapor (5) obtained by steam stripping of the third reactant flow enters a condenser to obtain gas-phase and liquid-phase products.
The catalytic cracking method for producing the low-carbon olefin by the Fischer-Tropsch synthetic oil disclosed by the invention is characterized in that the Fischer-Tropsch synthetic oil is hydrocarbon of which the carbon atom number is mainly 10-34 in a Fischer-Tropsch synthetic product.
According to the catalytic cracking method for producing the low-carbon olefin by using the Fischer-Tropsch synthetic oil, the diameter-expanding section of the lifting pipe is arranged above the catalyst inlet.
According to the catalytic cracking method for producing the low-carbon olefin by using the Fischer-Tropsch synthetic oil, the ratio of the diameter expansion section of the lifting pipe to the diameter of the lifting pipe is 1.2-2.0. The ratio of the length of the diameter-expanding section of the riser to the total length of the riser is 0.05-0.10.
According to the catalytic cracking method for producing the low-carbon olefin by using the Fischer-Tropsch synthetic oil, the aromatic raffinate oil is a fraction at 70-150 ℃, and the mass fraction of naphthenic hydrocarbon is not less than 50%.
According to the catalytic cracking method for producing the low-carbon olefin by using the Fischer-Tropsch synthetic oil, the Fischer-Tropsch synthetic oil accounts for 5-40% of the heavy oil by mass.
According to the catalytic cracking method for producing the low-carbon olefin by using the Fischer-Tropsch synthetic oil, the mass ratio of the aromatic raffinate oil to the heavy oil is 10-40%.
According to the catalytic cracking method for producing the low-carbon olefin by using the Fischer-Tropsch synthetic oil, the outlet temperature of the riser reactor is 540-610 ℃.
According to the catalytic cracking method for producing the low-carbon olefin by using the Fischer-Tropsch synthetic oil, the mass ratio of the regenerated catalyst to the heavy oil is (5).
Compared with the prior art, the invention has the following beneficial effects:
1. the invention realizes the improvement of the yield of the low-carbon olefin by utilizing the synergistic reaction of the Fischer-Tropsch synthesis oil and the aromatic raffinate oil in the catalytic cracking device, and simultaneously, the octane number of the gasoline is not reduced.
2. The invention only needs to simply transform the catalytic device, does not need to be subjected to a hydrogenation process, and has the characteristics of low investment, short flow, flexible operation and quick response.
Drawings
FIG. 1 is a process flow diagram of a catalytic cracking method for producing low-carbon olefins from Fischer-Tropsch synthetic oil.
Wherein: 1-Fischer-Tropsch synthesis oil feed inlet, 2-aromatic hydrocarbon raffinate oil feed inlet, 3-heavy oil feed inlet, 4-pre-lift gas, 5-mixed oil gas, 6-settler, 7-stripping reactor, 8-spent inclined tube, 9-regeneration inclined tube and 10-regenerator.
FIG. 2 is a process flow diagram of a riser catalytic cracking unit of the prior art.
In the drawings: 1-heavy oil feed inlet, 4-pre-lift gas, 5-mixed oil gas, 6-settler, 7-stripping reactor, 8-to-be-regenerated inclined tube, 9-regenerated inclined tube and 10-regenerator.
Detailed Description
The present invention will be described in further detail with reference to the accompanying drawings and specific embodiments. The drawings and detailed description do not limit the scope of the invention as claimed.
The main analysis method of the invention comprises the following steps:
in each of examples and comparative examples, na 2 O、Al 2 O 3 Chemical compositions such as these were measured by X-ray fluorescence (see "analytical methods of petrochemical industry (RIPP methods of experiments)", ed. Yang Cui et al, ed. Science publishers, published in 1990). The phase was determined by X-ray diffraction. The specific surface and the pore volume are measured by a low-temperature nitrogen adsorption-desorption method; the particle size distribution is analyzed by laser particle size (analysis method GB/T19077.1-2008); the abrasion index is determined by the abrasion index (straight tube method) (analytical method GB/T15458-1995); evaluation of Microreflective Activity (MA): the method of ASTM-D3907 was used. The catalyst adopts LDO-75 and propylene additive produced by catalyst factories of Lanzhou petrochemical company and is mixed according to a certain proportion.
The main raw materials and sources of the invention are as follows:
LDO-75 and propylene additive, produced by catalyst factories of Lanzhou petrochemical company, are subjected to hydrothermal deactivation treatment for 10 hours at the temperature of 800 ℃ and with 100 percent of water vapor before evaluation, and the physicochemical properties of the catalyst after hydrothermal aging are shown in Table 1.
TABLE 1 physicochemical Properties of the catalyst
The Fischer-Tropsch synthesis oil is from an Yan mine 100 ten thousand tons/year low-temperature Fischer-Tropsch synthesis device (properties are shown in a table 2), the aromatic raffinate oil is from a Lanzhou petrochemical 30 ten thousand tons/year aromatic extraction device (properties are shown in a table 3), the heavy oil is from a fresh catalytic raw material (properties are shown in a table 4, and the following is 300 ten thousand catalyst) of a Lanzhou petrochemical company 300 ten thousand tons/year catalytic cracking device, the mixing mass ratio of the vacuum wax oil and the vacuum residue in the fresh catalytic raw material is (6).
The composition of the cracked gas and the composition of the generated oil in the reaction product are obtained by analyzing a gas chromatograph (America Agilent GC 7890); the composition and octane number of the cracked gasoline were measured by a gas chromatograph (Warran CP3800, USA).
TABLE 2 Fischer-Tropsch Synthesis oil Properties
TABLE 3 Properties of aromatic raffinate oils
TABLE 4 Properties of heavy oils
Example 1
The experiment was carried out using the apparatus shown in FIG. 1, the ratio of the inside diameter of the riser expanded section to the inside diameter of the riser was 1.2, the ratio of the length of the riser expanded section to the total length of the riser was 0.08, and the pre-lift medium was nitrogen. After the device is purged, and after an oil inlet nozzle and the like are installed, adding a catalyst (LDO-75: propylene additive = 4).
The Fischer-Tropsch synthetic oil with the mass flow rate of 150g/h enters a riser reactor from a Fischer-Tropsch synthetic oil feeding hole (1), and is subjected to contact reaction with a catalytic cracking regenerated catalyst from a regenerated inclined tube (9) in a riser expanding section, wherein the temperature of the regenerated catalyst is 690 ℃, and the catalyst and oil gas after the Fischer-Tropsch synthetic oil reacts with the regenerated catalyst continuously move upwards to obtain a first reaction material flow; aromatic raffinate oil with the mass flow rate of 150g/h enters a riser reactor (11) from an aromatic raffinate oil inlet (2) and is in contact reaction with a first reactant flow, a catalyst and oil gas after the reaction continuously move upwards to obtain a second reactant flow, heavy oil with the mass flow rate of 1500g/h enters the riser reactor from a heavy oil inlet (3) above the aromatic raffinate oil inlet and is in contact reaction with the second reactant flow, and a product after the reaction and the catalyst continuously move upwards to obtain a third reactant flow; the outlet temperature of the reactor is 600 ℃, the mass ratio of the Fischer-Tropsch synthetic oil to the heavy oil is 1. The third reactant flow is input into a settler (6) for gas-solid separation, the carbon deposited catalyst is stripped through a stripping reactor (7) and then enters a spent inclined tube (8), the spent catalyst enters a regenerator (10) for regeneration, and the obtained regenerated catalyst enters a riser reactor through a regeneration inclined tube (9) for circular reaction; and the third reaction material flow is stripped, and then mixed oil gas (5) obtained by separation through a settler enters a condenser to obtain gas-phase and liquid-phase products. The test was performed in parallel twice and the average results were obtained, and the operation conditions and the evaluation results are shown in table 5.
Comparative example 1
After the conventional riser device shown in FIG. 2 is adopted for testing, the device is purged, and an oil inlet nozzle and the like are installed, a catalyst (LDO-75: propylene additive =4: 1) is added into a regeneration reactor, and raw oil is prepared to enter the device after the temperature of each temperature measuring point of the device is stable and the fluidization of the catalyst is stable.
Heavy oil with the mass flow rate of 1500g/h enters a riser reactor at a heavy oil feed inlet (1) and is subjected to contact reaction with a catalytic cracking regenerated catalyst from a regenerated inclined tube (9), the temperature of the regenerated catalyst is 690 ℃, the outlet temperature of the reactor is 540 ℃, and the catalyst-oil ratio is 9.31, and the reacted product and the catalyst move upwards to obtain a reactant flow; the carbon deposition catalyst is stripped through a stripping reactor (7), then enters a spent inclined tube (8) through a precipitator (6), the spent catalyst enters a regenerator (10) for regeneration, and the obtained regenerated catalyst enters a riser reactor through a regeneration inclined tube (9) for cyclic reaction; the reaction material flow is stripped by a stripping reactor (7), and then mixed oil gas (5) separated by a settler enters a condenser to obtain gas-phase and liquid-phase products. The test was performed in duplicate and the results averaged, and the operating conditions and the evaluation results are shown in table 5.
Comparative example 2
The experiment was carried out using the apparatus shown in FIG. 1, the ratio of the inside diameter of the riser expanded section to the inside diameter of the riser was 1.2, the ratio of the length of the riser expanded section to the total length of the riser was 0.08, and the pre-lift medium was nitrogen. After the purging of the device is finished, after the oil inlet nozzle and the like are installed, adding a catalyst (LDO-75: propylene additive =4: 1) into the regeneration reactor, and preparing raw oil to enter the device after the temperature of each temperature measuring point of the device is stable and the fluidization of the catalyst is stable.
Mass flow rate of 150g/h of N 2 The Fischer-Tropsch synthetic oil enters a riser reactor from a feed inlet (1) of Fischer-Tropsch synthetic oil, and is subjected to contact reaction with a catalytic cracking regenerated catalyst from a regenerated inclined tube (9) at an expanding section of the riser, wherein the temperature of the regenerated catalyst is 690 ℃, and the Fischer-Tropsch synthetic oil is subjected to Fischer-Tropsch synthesisThe catalyst and the oil gas after the reaction of the oil and the regenerated catalyst continuously move upwards to obtain a first reactant flow; mass flow rate of 150g/h of N 2 The method comprises the following steps of (1) enabling the aromatic raffinate oil to enter a riser reactor (11) from an aromatic raffinate oil inlet (2) and to be in contact reaction with a first reactant flow, enabling a catalyst and oil gas after reaction to continuously move upwards to obtain a second reactant flow, enabling mixed raw oil (Fischer-Tropsch synthetic oil: aromatic raffinate oil: heavy oil = 1; the reactor outlet temperature was 600 ℃. The third reactant flow is input into a settler (6) for gas-solid separation, the carbon deposited catalyst is stripped through a stripping reactor (7) and then enters a spent inclined tube (8), the spent catalyst enters a regenerator (10) for regeneration, and the obtained regenerated catalyst enters a riser reactor through a regeneration inclined tube (9) for circular reaction; and the third reaction material flow is stripped, and then mixed oil gas (5) obtained by separation through a settler enters a condenser to obtain gas-phase and liquid-phase products. The test was performed in parallel twice and the average results were obtained, and the operation conditions and the evaluation results are shown in table 5.
Example 2
The experiment was carried out using the apparatus shown in FIG. 1, the ratio of the inside diameter of the riser expanded section to the inside diameter of the riser was 1.2, the ratio of the length of the riser expanded section to the total length of the riser was 0.08, and the pre-lift medium was nitrogen. After the purging of the device is finished, after the oil inlet nozzle and the like are installed, adding a catalyst (LDO-75: propylene additive =4: 1) into the regeneration reactor, and preparing raw oil to enter the device after the temperature of each temperature measuring point of the device is stable and the fluidization of the catalyst is stable.
Fischer-Tropsch synthetic oil with the mass flow rate of 75g/h enters a riser reactor from a Fischer-Tropsch synthetic oil feeding hole (1), and is subjected to contact reaction with a catalytic cracking regenerated catalyst from a regenerated inclined tube (9) in a riser expanding section, the temperature of the regenerated catalyst is 690 ℃, and the catalyst and oil gas after the Fischer-Tropsch synthetic oil reacts with the regenerated catalyst continuously move upwards to obtain a first reactant flow; aromatic raffinate oil with the mass flow rate of 150g/h enters a riser reactor (11) from an aromatic raffinate oil inlet (2) and is in contact reaction with a first reactant flow, a catalyst and oil gas after the reaction continuously move upwards to obtain a second reactant flow, heavy oil with the mass flow rate of 1500g/h enters the riser reactor from a heavy oil inlet (3) above the aromatic raffinate oil inlet and is in contact reaction with the second reactant flow, and a product after the reaction and the catalyst continuously move upwards to obtain a third reactant flow; the outlet temperature of the reactor is 600 ℃, the mass ratio of the Fischer-Tropsch synthetic oil to the heavy oil is 0.5 to 10, and the mass ratio of the aromatic raffinate oil to the heavy oil is 1. The third reaction material flow is input into a settler (6) for gas-solid separation, the carbon deposition catalyst is stripped by a stripping reactor (7) and then enters a spent inclined tube (8), the spent catalyst enters a regenerator (10) for regeneration, and the obtained regenerated catalyst enters a riser reactor through a regeneration inclined tube (9) for cyclic reaction; the third reactant flow is stripped and then separated by a settler to obtain mixed oil vapor (5) which enters a condenser to obtain gas-phase and liquid-phase products. The test was performed in duplicate and the results averaged, and the operating conditions and the evaluation results are shown in Table 6.
Comparative example 3
The experiment was carried out using the apparatus shown in FIG. 1, the ratio of the inside diameter of the riser expanded section to the inside diameter of the riser was 1.2, the ratio of the length of the riser expanded section to the total length of the riser was 0.08, and the pre-lift medium was nitrogen. After the purging of the device is finished, after the oil inlet nozzle and the like are installed, adding a catalyst (LDO-75: propylene additive =4: 1) into the regeneration reactor, and preparing raw oil to enter the device after the temperature of each temperature measuring point of the device is stable and the fluidization of the catalyst is stable.
Fischer-Tropsch synthetic oil with the mass flow rate of 750g/h enters a riser reactor from a Fischer-Tropsch synthetic oil feeding hole (1), and is subjected to contact reaction with a catalytic cracking regenerated catalyst from a regenerated inclined tube (9) in a riser expanding section, the temperature of the regenerated catalyst is 690 ℃, and the catalyst and oil gas after the Fischer-Tropsch synthetic oil reacts with the regenerated catalyst continuously move upwards to obtain a first reactant flow; aromatic raffinate oil with the mass flow rate of 750g/h enters a riser reactor (11) from an aromatic raffinate oil inlet (2) and is in contact reaction with a first reactant flow, a catalyst and oil gas after the reaction continuously move upwards to obtain a second reactant flow, heavy oil with the mass flow rate of 1500g/h enters the riser reactor from a heavy oil inlet (3) above the aromatic raffinate oil inlet and is in contact reaction with the second reactant flow, and a product after the reaction and the catalyst continuously move upwards to obtain a third reactant flow; the outlet temperature of the reactor is 600 ℃, the mass ratio of the Fischer-Tropsch synthetic oil to the heavy oil is 5. The third reaction material flow is input into a settler (6) for gas-solid separation, the carbon deposition catalyst is stripped by a stripping reactor (7) and then enters a spent inclined tube (8), the spent catalyst enters a regenerator (10) for regeneration, and the obtained regenerated catalyst enters a riser reactor through a regeneration inclined tube (9) for cyclic reaction; the third reactant flow is stripped and then separated by a settler to obtain mixed oil vapor (5) which enters a condenser to obtain gas-phase and liquid-phase products. The test was performed in parallel twice and the average results were obtained, and the operation conditions and the evaluation results are shown in table 6.
Example 3
The experiment was carried out using the apparatus shown in FIG. 1, the ratio of the inside diameter of the riser expanded section to the inside diameter of the riser was 1.2, the ratio of the length of the riser expanded section to the total length of the riser was 0.08, and the pre-lift medium was nitrogen. After the device is purged, and after an oil inlet nozzle and the like are installed, adding a catalyst (LDO-75: propylene additive = 4).
The Fischer-Tropsch synthetic oil with the mass flow rate of 300g/h enters a riser reactor from a Fischer-Tropsch synthetic oil feeding hole (1), and is subjected to contact reaction with a catalytic cracking regenerated catalyst from a regenerated inclined tube (9) in a riser expanding section, the temperature of the regenerated catalyst is 690 ℃, and the catalyst and oil gas after the Fischer-Tropsch synthetic oil reacts with the regenerated catalyst continuously move upwards to obtain a first reactant flow; aromatic raffinate oil with the mass flow rate of 300g/h enters a riser reactor (11) from an aromatic raffinate oil inlet (2) and is in contact reaction with a first reactant flow, a catalyst and oil gas after the reaction continuously move upwards to obtain a second reactant flow, heavy oil with the mass flow rate of 1500g/h enters the riser reactor from a heavy oil inlet (3) above the aromatic raffinate oil inlet and is in contact reaction with the second reactant flow, and a product after the reaction and the catalyst continuously move upwards to obtain a third reactant flow; the outlet temperature of the reactor is 600 ℃, the mass ratio of the Fischer-Tropsch synthetic oil to the heavy oil is 2. The third reactant flow is input into a settler (6) for gas-solid separation, the carbon deposited catalyst is stripped through a stripping reactor (7) and then enters a spent inclined tube (8), the spent catalyst enters a regenerator (10) for regeneration, and the obtained regenerated catalyst enters a riser reactor through a regeneration inclined tube (9) for circular reaction; and the third reaction material flow is stripped, and then mixed oil gas (5) obtained by separation through a settler enters a condenser to obtain gas-phase and liquid-phase products. The test was performed in duplicate and the results averaged, and the operating conditions and the evaluation results are shown in Table 7.
Comparative example 4
The apparatus shown in FIG. 1 was used for the test, the ratio of the inner diameter of the riser expanding section to the inner diameter of the riser was 1.2, the ratio of the length of the riser expanding section to the total length of the riser was 0.08, and the pre-lift medium was nitrogen. After the device is purged, and after an oil inlet nozzle and the like are installed, adding a catalyst (LDO-75: propylene additive = 4).
The Fischer-Tropsch synthetic oil with the mass flow rate of 300g/h enters a riser reactor from a Fischer-Tropsch synthetic oil feeding hole (1), and is subjected to contact reaction with a catalytic cracking regenerated catalyst from a regenerated inclined tube (9) in a riser expanding section, wherein the temperature of the regenerated catalyst is 690 ℃, and the catalyst and oil gas after the Fischer-Tropsch synthetic oil reacts with the regenerated catalyst continue to move upwards to obtain a first reaction material flow; aromatic raffinate oil with the mass flow rate of 300g/h enters a riser reactor (11) from an aromatic raffinate oil inlet (2) and is in contact reaction with a first reactant flow, a catalyst and oil gas after the reaction continuously move upwards to obtain a second reactant flow, heavy oil with the mass flow rate of 1500g/h enters the riser reactor from a heavy oil inlet (3) above the aromatic raffinate oil inlet and is in contact reaction with the second reactant flow, and a product after the reaction and the catalyst continuously move upwards to obtain a third reactant flow; the outlet temperature of the reactor is 530 ℃, the mass ratio of the Fischer-Tropsch synthesis oil to the heavy oil is 2. The third reaction material flow is input into a settler (6) for gas-solid separation, the carbon deposition catalyst is stripped by a stripping reactor (7) and then enters a spent inclined tube (8), the spent catalyst enters a regenerator (10) for regeneration, and the obtained regenerated catalyst enters a riser reactor through a regeneration inclined tube (9) for cyclic reaction; the third reactant flow is stripped and then separated by a settler to obtain mixed oil vapor (5) which enters a condenser to obtain gas-phase and liquid-phase products. The test was performed in parallel twice and the average results were obtained, and the operation conditions and the evaluation results are shown in table 7.
Table 5 reaction conditions and reaction results of example 1 and comparative examples 1 and 2
Table 6 reaction conditions and reaction results of example 2 and comparative example 3
Table 7 reaction conditions and reaction results of example 3 and comparative example 4
As can be seen from Table 5, the yield of liquefied gas is increased after blending 10% Fischer-Tropsch synthetic oil and 10% aromatic raffinate oil; example 1 using the process of the present invention increased the triene (ethylene + propylene + butylene) yield by 3.67 units and slightly increased the gasoline RON compared to comparative example 2 using a mixed feed with heavy oil. The triene yield increased by 7.34 units and the gasoline RON increased compared to comparative example 1 under conventional reaction conditions.
As can be seen from Table 6, when the amount of the Fischer-Tropsch synthetic oil and the aromatic raffinate oil is more than 40%, higher triene yield can be obtained, but the reduction of the RON of the gasoline is larger. As can be seen from table 7, the higher reaction temperature promoted the production of liquefied gas, and greatly increased the triene yield, but when the reaction temperature was 540 ℃, the triene yield was lower, and the RON of gasoline was also reduced.
In conclusion, the catalytic cracking method for producing the low-carbon olefin from the Fischer-Tropsch synthetic oil provided by the invention utilizes the synergistic reaction of the Fischer-Tropsch synthetic oil and the aromatic raffinate oil in the catalytic cracking device, so that the yield of liquefied gas is higher, the yield of the low-carbon olefin is higher, and the octane number of gasoline is not reduced. The invention only needs to simply transform the catalytic device, does not need to carry out hydrogenation process, and has the characteristics of less investment, short flow, flexible operation and quick response.
Claims (13)
1. The catalytic cracking method for producing the low-carbon olefin by using the Fischer-Tropsch synthetic oil is characterized by comprising the following steps of:
step (1): inputting Fischer-Tropsch synthetic oil into a riser reactor, and carrying out contact reaction on the Fischer-Tropsch synthetic oil and a catalytic cracking regenerated catalyst at an expanding section of the riser reactor to obtain a first reaction material flow;
step (2): inputting aromatic hydrocarbon raffinate oil into a riser reactor from the top of an expanding section, and carrying out contact reaction with a first reactant flow to obtain a second reactant flow;
and (3): inputting heavy oil into the riser reactor above the aromatics raffinate oil inlet, and allowing the heavy oil to contact and react with the second reactant flow to obtain a third reactant flow;
and (4): stripping the carbon deposition catalyst in the third reaction material flow through a stripping reactor, then entering a to-be-regenerated inclined tube through a settler, entering a regenerator for regeneration, and entering an obtained regenerated catalyst into a riser reactor for cyclic reaction; and the mixed oil steam obtained after the third reactant flow is stripped enters a condenser to obtain a gas-phase product and a liquid-phase product.
2. The catalytic cracking method for producing low carbon olefins from Fischer-Tropsch synthesis oil according to claim 1, wherein the Fischer-Tropsch synthesis oil is hydrocarbons of C10-C34 in Fischer-Tropsch synthesis products.
3. The catalytic cracking method for producing low carbon olefins from Fischer-Tropsch synthesis oil according to claim 1, wherein the riser reactor is provided with a pre-lifting section and an expanding section in sequence from bottom to top along the vertical direction, and the lifting and expanding section is positioned above the catalyst inlet.
4. The catalytic cracking method for producing low carbon olefins from Fischer-Tropsch synthesis oil according to claim 3, wherein the ratio of the diameter of the expanding section to the diameter of the pre-lifting section is 1.2-2.0.
5. The catalytic cracking method for producing low carbon olefins from Fischer-Tropsch synthesis oil according to claim 1, wherein the ratio of the length of the expanding section to the total length of the riser reactor is 0.05-0.10.
6. The catalytic cracking method for producing low carbon olefins from Fischer-Tropsch synthesis oil according to claim 1, wherein the aromatic raffinate oil is a petroleum hydrocarbon fraction at 70-150 ℃, and the naphthenic hydrocarbon content of the aromatic raffinate oil is not less than 50% by mass.
7. The catalytic cracking method for producing low carbon olefins from Fischer-Tropsch synthesis oil according to claim 1 or 6, wherein the heavy oil is slurry oil produced by a catalytic cracking process, and is at least one of heavy fraction and straight run vacuum fraction produced by coking, thermal cracking and visbreaking processes.
8. The catalytic cracking method for producing low carbon olefins from Fischer-Tropsch synthesis oil according to claim 1, wherein the micro-reaction activity of the regenerated catalyst is 55-75%.
9. The catalytic cracking method for producing low-carbon olefins from Fischer-Tropsch synthetic oil according to claim 1, wherein the Fischer-Tropsch synthetic oil accounts for 5-40% of the heavy oil by mass.
10. The catalytic cracking method for producing low carbon olefins from Fischer-Tropsch synthesis oil according to claim 1, wherein the mass ratio of the aromatic raffinate oil to the heavy oil is 10-40%.
11. The catalytic cracking method for producing low carbon olefins from Fischer-Tropsch synthesis oil according to claim 1, wherein the Fischer-Tropsch synthesis oil and the aromatic raffinate oil are used in the same amount or different amounts.
12. The catalytic cracking method for producing low carbon olefins from Fischer-Tropsch synthesis oil according to claim 1, wherein the outlet temperature of the riser reactor is 540-610 ℃.
13. The catalytic cracking method for producing the low-carbon olefins from the Fischer-Tropsch synthesis oil according to claim 1, wherein the mass ratio of the regenerated catalyst to the heavy oil is (5).
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| CN102533322A (en) * | 2010-12-30 | 2012-07-04 | 中国石油化工股份有限公司 | Method for producing propylene by using Fischer Tropsch synthetic oil in catalytic cracking mode |
| CN105622316A (en) * | 2014-10-29 | 2016-06-01 | 中国石油化工股份有限公司 | Conversion method of Fischer-Tropsch synthesis oil raw material |
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| CN101531558A (en) * | 2008-03-13 | 2009-09-16 | 中国石油化工股份有限公司 | Catalytic conversion method for preparing propylene and aromatic hydrocarbons |
| CN102533322A (en) * | 2010-12-30 | 2012-07-04 | 中国石油化工股份有限公司 | Method for producing propylene by using Fischer Tropsch synthetic oil in catalytic cracking mode |
| CN105622316A (en) * | 2014-10-29 | 2016-06-01 | 中国石油化工股份有限公司 | Conversion method of Fischer-Tropsch synthesis oil raw material |
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