CN101928588B - Catalytic conversion method of hydrocarbon oil - Google Patents
Catalytic conversion method of hydrocarbon oil Download PDFInfo
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Abstract
A catalytic conversion method of hydrocarbon oil comprises the following steps: leading the mixture of preheated light hydrocarbon oil and heavy hydrocarbon oil in a reactor from the bottom to contact a catalyst from a regenerator to carry out catalytic cracking reaction, the mixture and the catalyst flowing upward together, leading the reaction product and a spent catalyst with coke out of the reactor from an outlet on the upper part of the reactor, the reaction product and the spent catalyst entering into an oiling agent separation system, recycling the separated catalyst after stripping, burning and regenerating and the separated reaction oil and gas entering into a subsequent separation system to separate the product. The method provided by the invention can obviously reduce the yieldof the coke, greatly increase the yields of diesel and liquefied gas, simultaneously reduce the yield of dry gas and obviously improve the quality of the gasoline.
Description
Technical field
The invention belongs under the situation that does not have hydrogen the catalytic cracking of hydrocarbon ils.Specifically, the present invention is that a kind of mixture with light hydrocarbon oil and heavy hydrocarbon oil is the catalyst cracking method of raw material.
Background technology
Catalytic cracking is one of important technical of heavy oil lighting, along with crude oil heaviness and poor qualityization, and the light-end products demand increased day by day, the catalytically cracked stock source constantly enlarges, and the heaviness of catalytically cracked stock and poor qualityization are also in continuous aggravation.Because catalytic cracking reaction and heat cracking reaction are to take place together in catalytic cracking process, particularly after stock oil heaviness and poor qualityization, the mobile variation of raw material, the atomizing effect variation, raw material is in catalyst surface and hole internal diffusion degradation, cause part material to be converted into coke in the catalyzer deposition, the catalytic cracking reaction coke yield is obviously increased.
CN101215476A discloses a kind of assistant for catalytic cracking coking-inhibiting yield-increasing for catalytic cracking (FCC) device, and is good with the catalytic cracking media compatibility, can improve the intermingled dregs ratio of FCC apparatus after the adding, improves yield of light oil and reduces coke yield.
CN101144030A discloses a kind of catalyst cracking method, it is characterized in that one or more ionic liquids are added in the stock oil as auxiliary agent, and add-on is to account for 10 heavy～10000ppm of stock oil.This method can improve the mink cell focus conversion capability especially, reduces slurry oil, increases yield of light oil, suppresses green coke.
CN1680515A discloses a kind of catalytic cracking microexplosion activator, it comprises high performance tensio-active agent, water, catalyst activator, before the catalytic cracking riser nozzle, mix with raw material, by moisture and absorb the water-in-oil microemulsion liquid that water in the raw material forms the nano level yardstick, contact the generation microexplosion with high temperature catalyst, improve atomizing effect, produce the hydrocarbon fragment of band reactive hydrogen, activating element is adsorbed onto on the catalyzer, improve catalyst activity, reduce catalyst contamination, reach and improved gasoline+solar oil+yield of liquefied gas, productivity of propylene, ethene+propylene+total butylene productive rate, hydrogen sulfide content and reduction coke productive rate in the dry gas, hydrogen yield, hydrogen methane, reduce the purpose of sulfur in gasoline alcohol content.
CN1160746A discloses a kind of catalysis conversion method that improves low-quality gasoline fraction octane value, be characterized in injecting low octane value gasoline at any position, the bottom of the cracking stock inlet end of catalytic cracking riser reactor, it is contacted with high temperature catalyst from revivifier.The gasoline upgrading reaction takes place under the certain reaction condition, the mixture that contains micro-coke and reaction oil gas that generates upwards promotes, contact with the cracking stock that sprays into, reaction generates reclaimable catalyst and the reaction oil gas mixture that contains charcoal under cracking conditions, separates then, regenerates again.
Summary of the invention
The invention provides a kind of catalysis conversion method of hydrocarbon ils, this method is raw material with the mixture of light hydrocarbon oil and heavy hydrocarbon oil, carries out catalytic cracking, can significantly reduce the coke productive rate, increases diesel oil and liquefied gas yield simultaneously.
A kind of catalysis conversion method of hydrocarbon ils, comprise the light hydrocarbon oil of preheating and the mixture of heavy hydrocarbon oil, introduce reactor by the bottom, contact with the catalyzer that comes from revivifier and to carry out catalytic cracking reaction, and upwards flow together, reaction product is drawn reactor with the reclaimable catalyst of band coke by top exit, entering the finish separation system separates, isolated catalyzer enters the revivifier coke burning regeneration behind stripping, regenerated catalyst Returning reactor bottom recycles, isolated reaction oil gas enters subsequent separation system, product separation; Described light hydrocarbon oil is that boiling range is 30～220 ℃ petroleum hydrocarbon cut, and described heavy hydrocarbon oil is the petroleum hydrocarbon cut of initial boiling point 〉=250 ℃, and the mass ratio of light hydrocarbon oil and heavy hydrocarbon oil is 0.01～0.8: 1.
The mass ratio of light hydrocarbon oil and heavy hydrocarbon oil is preferably 0.05～0.5: 1.
Described light hydrocarbon oil is preferably one or more the mixture in the naphtha fraction of technologies such as crude oil atmospheric distillation, mink cell focus catalytic cracking, mink cell focus thermally splitting, viscosity breaking, delayed coking, heavy oil hydrocracking, hydrotreatment, hydrofining.
Described heavy hydrocarbon oil is preferably vacuum residue fraction, long residuum or vacuum residuum solvent-deasphalted oils, long residuum or the vacuum residuum hydrocracking tail oil of decompressed wax oil cut, the crude oil underpressure distillation of long residuum cut, the crude oil underpressure distillation of crude oil atmospheric distillation, one or more the mixture in the mink cell focus hydrotreatment heavy oil fraction.
Described catalyzer is catalytic cracking catalyst, can contain or not contain molecular sieve.Molecular sieve is optional self-contained or do not contain the Y of rare earth or in HY type zeolite, the ultrastable Y that contains or do not contain rare earth, ZSM-5 series zeolite, the supersiliceous zeolite with five-membered ring structure, β zeolite and the ferrierite one or more; The catalytic cracking catalyst that does not contain molecular sieve is the amorphous silicon aluminium catalyzer.
Described reactor is fluidized-bed reactor or riser reactor.
When described reactor is riser reactor, reaction conditions is: temperature of reaction is 450～650 ℃, reaction pressure is 100～450KPa, catalyzer is 1～25: 1 with raw materials quality than (agent-oil ratio), the mass ratio of atomized water steam and stock oil (water-oil ratio) is 0.01～0.3: 1, and the reaction times is 0.1～30 second.Preferred reaction conditions is: temperature of reaction is 480～550 ℃, and reaction pressure is 100～300KPa, and catalyzer is 3～15: 1 with the raw materials quality ratio, and the mass ratio of atomized water steam and stock oil is 0.05～0.2: 1, and the reaction times is 0.1～10 second.
When described reactor is fluidized-bed reactor, reaction conditions is: temperature of reaction is 450～650 ℃, and reaction pressure is 100～450KPa, and catalyzer is 1～25: 1 with the raw materials quality ratio, the mass ratio of atomized water steam and stock oil is 0.01～0.3: 1, and weight hourly space velocity is 1～100h
-1Preferred reaction conditions is: temperature of reaction is 480～550 ℃, and reaction pressure is 100～300KPa, and catalyzer is 3～15: 1 with the raw materials quality ratio, and the mass ratio of atomized water steam and stock oil is 0.05～0.2: 1, and weight hourly space velocity is 2～50h
-1
Useful technique effect of the present invention is: adopt method of the present invention, can significantly reduce coke yield, increase substantially diesel oil and liquefied gas yield, reduce dry gas yied simultaneously, and can significantly improve gasoline quality.In addition, adopt method of the present invention to be conducive to improve the ratio that catalytic cracking unit is mixed refining vacuum residuum.
Embodiment
Below concrete set forth the present invention.
With the light hydrocarbon oil of preheating and the mixture of heavy hydrocarbon oil, introduce reactor by the bottom, in the presence of the lifting medium, upwards flow, contact with the high temperature catalyst that comes from revivifier and to carry out catalytic cracking reaction, reaction product is drawn by the reactor head outlet with the reclaimable catalyst of band coke, entering the finish separation system separates, isolated catalyzer enters the revivifier coke burning regeneration behind stripping, recycle, the stripper service temperature is 400～650 ℃, the mass ratio of water vapor and reclaimable catalyst is 0.1～1: 1, and the temperature of burning of revivifier is 600～780 ℃; Isolated reaction oil gas enters subsequent separation system, separates fluid
Products such as gasification, gasoline, diesel oil.
Described catalyzer is catalytic cracking catalyst, can adopt any method of the prior art to prepare.Gross weight with catalyzer is benchmark, and described catalyzer preferably includes the molecular sieve of 5～50wt%, the aluminum oxide of 5～70wt% and the silicon oxide of surplus, more preferably comprises the molecular sieve of 20～45wt%, the aluminum oxide of 25～50wt% and the silicon oxide of surplus.During above-mentioned catalyst chemical is formed, molecular sieve be add in the preparation process or preparation process in form through crystallization, aluminum oxide and silicon oxide derive from inorganic oxide binder and clay.
Described molecular screening is self-contained or do not contain the Y of rare earth or in HY type zeolite, the ultrastable Y that contains or do not contain rare earth, ZSM-5 series zeolite, the supersiliceous zeolite with five-membered ring structure, β zeolite and the ferrierite one or more.
Described clay is conventionally known to one of skill in the art, is preferably kaolin, metakaolin, sepiolite, attapulgite, montmorillonite and tiredly takes off in the stone one or more.
Described inorganic oxide binder is conventionally known to one of skill in the art, is preferably in pseudo-boehmite, aluminium colloidal sol, silicon sol, water glass and the phosphorus aluminium colloidal sol one or more.
Described light hydrocarbon oil is that boiling range is 30～220 ℃ petroleum hydrocarbon cut, the mixture of one or more that can be crude oil in petroleum naphtha (boiling range is 30～220 ℃) that time processing is produced, petroleum naphtha, light naphthar (boiling range is 30～100 ℃) fraction, heavy naphtha (boiling range is 100～220 ℃) through secondary processing is produced.Described time processing is crude oil atmospheric distillation, and described secondary processing comprises catalytic cracking, thermally splitting, viscosity breaking, delayed coking, hydrocracking, hydrotreatment, hydrofining etc.
Described heavy hydrocarbon oil is the petroleum hydrocarbon cut of initial boiling point 〉=250 ℃, is preferably vacuum residue fraction, long residuum or vacuum residuum solvent-deasphalted oils, long residuum or the vacuum residuum hydrocracking tail oil of decompressed wax oil cut, the crude oil underpressure distillation of long residuum cut, the crude oil underpressure distillation of crude oil atmospheric distillation, one or more the mixture in the mink cell focus hydrotreatment heavy oil fraction.
Described reactor is fluidized-bed reactor or riser reactor.Wherein, riser reactor can be cylindrical reactor, and namely each section diameter is identical, also can be the reducing reactor, the visible Chinese patent CN10478094C of concrete reactor types, CN1091393C.
When described reactor is riser reactor, reaction conditions is: temperature of reaction is 450～650 ℃, and reaction pressure is 100～450KPa, and catalyzer is 1～25: 1 with the raw materials quality ratio, the mass ratio of atomized water steam and stock oil is 0.01～0.3: 1, and the reaction times is 0.1～30 second.Preferred reaction conditions is: temperature of reaction is 480～550 ℃, and reaction pressure is 100～300KPa, and catalyzer is 3～15: 1 with the raw materials quality ratio, and the mass ratio of atomized water steam and stock oil is 0.05～0.2: 1, and the reaction times is 0.1～10 second.
When described reactor is fluidized-bed reactor, the catalytic cracking reaction condition is: temperature of reaction is 450～650 ℃, and reaction pressure is 100～450KPa, and catalyzer is 1～25: 1 with the raw materials quality ratio, the mass ratio of atomized water steam and stock oil is 0.01～0.5: 1, and weight hourly space velocity is 1～100h
-1Preferred reaction conditions is: temperature of reaction is 480～550 ℃, and reaction pressure is 100～300KPa, and catalyzer is 3～15: 1 with the raw materials quality ratio, and the mass ratio of atomized water steam and stock oil is 0.05～0.3: 1, and weight hourly space velocity is 2～50h
-1
Further specify the present invention by the following examples.
Catalytic cracking catalyst MLC-500 used among Comparative Examples and the embodiment is produced by catalyzer branch office of China PetroChemical Corporation Shandong catalyst plant, and its character is listed in table 1; Used catalytic cracking petroleum naphtha, the character of straight-run spirit are listed in table 2, and the character of long residuum is listed in table 3.
Comparative Examples 1
The product of Comparative Examples explanation long residuum catalytic cracking distributes and gasoline products character.
MLC-500 is packed in the reactor of fixed fluidized bed reaction unit, and loaded catalyst is 240g.Through entering reactor after the preheater heating with after atomizing steam mixes, with the high temperature catalyst reaction, the oil gas of generation is collected reacted gas and liquid product respectively after three grades of coolings in reactor with long residue feed.Surface deposition the reclaimable catalyst of coke feed the excess air high temperature regeneration, volume and the liquid product weight of metering flue gas, reacted gas.Experiment condition is: oil inlet quantity 40g, oil-feed time 120s, 100 ℃ of preheating temperatures, 510 ℃ of temperature of reaction, agent-oil ratio 6, air speed 4h
-1, the results are shown in table 4, gasoline property is listed in table 5.
Embodiment 1～2 explanation method provided by the invention distributes and gasoline products character for long residuum mixes the product that carries out catalytic cracking reaction in the back under the condition identical with Comparative Examples with catalytically cracked gasoline, straight-run spirit respectively.
Embodiment 1
MLC-500 is packed in the reactor of fixed fluidized bed reaction unit, and loaded catalyst is 240g.Long residue feed and catalytically cracked gasoline are entered reactor by 95: 5 mixed by preheater heating back and after atomizing steam mixes, with the high temperature catalyst reaction, the oil gas of generation is collected reacted gas and liquid product respectively after three grades of coolings in reactor.Surface deposition the reclaimable catalyst of coke feed the excess air high temperature regeneration, volume and the liquid product weight of metering flue gas, reacted gas.Experiment condition is: oil inlet quantity 40g, oil-feed time 120s, 100 ℃ of preheating temperatures, 510 ℃ of temperature of reaction, agent-oil ratio 6, air speed 4h
-1, the results are shown in table 4, gasoline property is listed in table 5.
Embodiment 2
MLC-500 is packed in the reactor of fixed fluidized bed reaction unit, and loaded catalyst is 240g.Long residue feed and straight-run spirit are entered reactor by 85: 15 mixed by preheater heating back and after atomizing steam mixes, with the high temperature catalyst reaction, the oil gas of generation is collected reacted gas and liquid product respectively after three grades of coolings in reactor.Surface deposition the reclaimable catalyst of coke feed the excess air high temperature regeneration, volume and the liquid product weight of metering flue gas, reacted gas.Experiment condition is: oil inlet quantity 40g, oil-feed time 120s, 100 ℃ of preheating temperatures, 510 ℃ of temperature of reaction, agent-oil ratio 6, air speed 4h
-1, the results are shown in table 4, gasoline property is listed in table 5.
Comparative Examples 2
This Comparative Examples adopts medium-sized riser reactor, and this riser reactor is that total height is 10 meters, and diameter is 25 centimetres cylindrical structure, and this riser tube foot is pre lift zone.Catalyzer uses the MLC-500 of table 1, and the raw material of processing is the long residuum of table 3.
Concrete implementation step is: the long residuum after the preheating enters the riser reactor bottom by atomizing nozzle, mix with the regenerated catalyst from revivifier under the effect of pre-lifting medium, upwards to the riser reactor outlet, enter settling vessel along riser tube, separating catalyst and reaction product, reaction product enters the subsequent separation system product separation, catalyzer obtains reclaimable catalyst through the stripper stripping, and reclaimable catalyst enters and recycles after revivifier burns the recovery activity.
Main operational condition is: 675 ℃ of regenerator temperature, 505 ℃ of riser tube temperature outs, 170 kPas of pressure, 180 ℃ of raw material preheating temperatures, the atomizing steam amount is 6% of stock oil, pre-lifting quantity of steam is 5% of raw material stock oil, agent-oil ratio 6, stock oil 4 seconds residence time (reaction times) in riser tube.
The results are shown in table 6, gasoline property is listed in table 7.
Embodiment 3
Repeat the test of Comparative Examples 2, difference is that stock oil is the mixture of long residuum and catalytically cracked gasoline.The results are shown in table 6, gasoline property is listed in table 7.
Embodiment 4
Repeat the test of embodiment 3, difference is that stock oil is the mixture of long residuum and straight-run spirit.The results are shown in table 6, gasoline property is listed in table 7.
Table 1
Table 2
Table 3
Table 4
By table 4 as seen, adopt method provided by the invention to carry out catalytic cracking reaction, can significantly reduce coke yield, can increase diesel oil and liquefied gas yield simultaneously.
Table 5
As seen from Table 5, adopt method provided by the invention to carry out catalytic cracking reaction, can significantly reduce content of olefin in gasoline and sulphur content, significantly improved the quality of gasoline products.
Table 6
By table 6 as seen, adopt method provided by the invention to carry out catalytic cracking reaction, can significantly reduce coke yield, can increase diesel oil and liquefied gas yield simultaneously.
Table 7
As seen from Table 7, adopt method provided by the invention to carry out catalytic cracking reaction, can significantly reduce content of olefin in gasoline and sulphur content, significantly improved the quality of gasoline products.
Claims (8)
1. the catalysis conversion method of a hydrocarbon ils, comprise the light hydrocarbon oil of preheating and the mixture of heavy hydrocarbon oil, introduce reactor by the bottom, contact with the high temperature catalyst that comes from revivifier and to carry out catalytic cracking reaction, and upwards flow together, reaction product is drawn reactor with the reclaimable catalyst of band coke by top exit, entering the finish separation system separates, isolated catalyzer enters the revivifier coke burning regeneration behind stripping, regenerated catalyst Returning reactor bottom recycles, isolated reaction oil gas enters subsequent separation system, product separation; Described light hydrocarbon oil is that boiling range is 30～220 ℃ petroleum hydrocarbon cut, and described heavy hydrocarbon oil is the petroleum hydrocarbon cut of initial boiling point 〉=250 ℃, and the mass ratio of light hydrocarbon oil and heavy hydrocarbon oil is 0.01～0.8: 1; Described catalyzer is catalytic cracking catalyst.
2. in accordance with the method for claim 1, it is characterized in that the mass ratio of light hydrocarbon oil and heavy hydrocarbon oil is 0.05～0.5: 1.
3. in accordance with the method for claim 1, it is characterized in that described light hydrocarbon oil is one or more the mixture in crude oil atmospheric distillation, mink cell focus catalytic cracking, mink cell focus thermally splitting, viscosity breaking, delayed coking, heavy oil hydrocracking, hydrotreatment, the hydrorefined naphtha fraction.
4. in accordance with the method for claim 1, it is characterized in that described heavy hydrocarbon oil is vacuum residue fraction, long residuum or vacuum residuum solvent-deasphalted oils, long residuum or the vacuum residuum hydrocracking tail oil of decompressed wax oil cut, the crude oil underpressure distillation of long residuum cut, the crude oil underpressure distillation of crude oil atmospheric distillation, one or more the mixture in the mink cell focus hydrotreatment heavy oil fraction.
5. in accordance with the method for claim 1, it is characterized in that, described reactor is riser reactor, reaction conditions is: temperature of reaction is 450～650 ℃, reaction pressure is 100～450KPa, catalyzer is 1～25: 1 with the raw materials quality ratio, and the mass ratio of atomized water steam and stock oil is 0.01～0.3: 1, and the reaction times is 0.1～30 second.
6. in accordance with the method for claim 5, it is characterized in that temperature of reaction is 480～550 ℃, reaction pressure is 100～300KPa, catalyzer is 3～15: 1 with the raw materials quality ratio, and the mass ratio of atomized water steam and stock oil is 0.05～0.3: 1, and the reaction times is 0.1～10 second.
7. in accordance with the method for claim 1, it is characterized in that, described reactor is fluidized-bed reactor, reaction conditions is: temperature of reaction is 450～650 ℃, reaction pressure is 100～450KPa, catalyzer is 1～25: 1 with the raw materials quality ratio, and the mass ratio of atomized water steam and stock oil is 0.01～0.3: 1, and weight hourly space velocity is 1～100h
-1
8. in accordance with the method for claim 7, it is characterized in that reaction conditions is: temperature of reaction is 480～550 ℃, reaction pressure is 100～300KPa, catalyzer is 3～15: 1 with the raw materials quality ratio, and the mass ratio of atomized water steam and stock oil is 0.05～0.3: 1, and weight hourly space velocity is 2～50h
-1
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