CN101343568A - Method for preparing gasoline with petroleum cracking of dry gas - Google Patents
Method for preparing gasoline with petroleum cracking of dry gas Download PDFInfo
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- CN101343568A CN101343568A CNA2008100841266A CN200810084126A CN101343568A CN 101343568 A CN101343568 A CN 101343568A CN A2008100841266 A CNA2008100841266 A CN A2008100841266A CN 200810084126 A CN200810084126 A CN 200810084126A CN 101343568 A CN101343568 A CN 101343568A
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Abstract
Disclosed is a method for producing gasoline by petroleum cracking dry gases, which is characterized in that the petroleum catalytic cracking dry gases of a catalytic cracking dry gas, a deep catalytic cracking (DCC) dry gas, a coking dry gas and the like are input to a reactor filled with catalyst for reaction to generate gasoline at a reaction temperature of 200 DEG C to 500 DEG C, a reaction pressure of between 0.1 MPa and 1.0 MPa, and a volume space velocity ranging from 100 h<-1> to 2000 h<-1>.
Description
Technical field
The present invention relates to effective utilization of petroleum cracking dry gas, can promote the dry gas economic worth.The dry gas source comprises catalytic cracked dry gas, catalytic pyrolysis (DCC) dry gas, coking dry gas etc.Product is based on gasoline.
Background technology
Whole world petroleum resources worsening shortages, the high-order operation of oil price, how making good use of limited resources becomes one of problem that oil refining enterprise need solve.Catalytic cracking is the main operating unit of refinery, and effect is huge aspect processing heavy oil.The catalyzed cracking processing amount is very big, accounts for about 35% of crude oil time processing amount.At present, domestic catalyzed cracking processing ability is above 100,000,000 tons.Catalytic cracking production comprises dry gas, liquefied gas, gasoline, diesel oil, slurry oil, coke etc., and in these products, dry gas is worth lower, is undesirable product.The dry gas mass yield is approximately 4%～8% of charging, its typical volume consists of: hydrogen 20～40%, methane 15～30%, ethane 10～15%, ethene 10～20%, propane, propylene and heavy constituent 0.5～3%, nitrogen 5～15% contains a small amount of carbon monoxide, carbonic acid gas in addition.Concerning a cover working ability is 1,000,000 tons/year catalytic cracking unit, about 0.1 ten thousand tons/year of hydrogen, about 1.0 ten thousand tons/year of ethene, about 0.15 ten thousand tons/year of propylene in the dry gas.
Present most of refinery uses the dry gas gas that acts as a fuel, and has obviously caused very big waste.Because contain higher hydrogen of a large amount of value and ethene in the dry gas, how utilizing hydrogen and ethene in the dry gas is to improve the key that dry gas is worth.
Hydrogen in the extraction separation dry gas is a direction.A kind of method as CN1184136C just provides.Utilize dry gas to produce hydrogen, economic benefit is fair, but produces in the hydrogen technological process, needs unit such as purification, hydrogenation, steam reforming, conversion, separation, complicated operating process.The method of a kind of oil refinery dry gas selective oxidation catalyzing manufacturing of hydrogen that CN1095440C discloses, though saved the hydrogenation unit operation, this method has been introduced oxygen-containing gas.If introducing air, then a nitrogen content is higher in the product gas; If introducing oxygen then needs air separation facility to cooperate.
Extracting ethene from catalytic cracked dry gas is to promote another approach that dry gas is worth.Recent technology mainly contains separation by deep refrigeration, absorption extraction method, hydrate partition method, membrane separation process and adsorption method of separation, and wherein separation by deep refrigeration, absorption extraction method are quite ripe, and have realized suitability for industrialized production, but both all need certain energy consumption.Adsorption separating method needs transformation absorption, wet desulphurization decarburization, faces complete sets of Techniques operations such as hydrogen deoxidation, aluminum oxide and molecular sieve drying, and process is more complicated also.Membrane separation process and adsorption method of separation are in laboratory study or commerical test stage.
Utilize ethene and benzene reaction properties in the dry gas, produce vinylbenzene, be utilize dry gas than good method, these class methods have full scale plant production.
The inventor finds that unexpectedly dry gas can be converted into gasoline.It happened like this, the inventor is in the technical process of research dry gas selective adsorption separating hydrogen gas and ethene, when optimizing the test of investigating various sorbent materials, once in the test, staff's mishandle, become 400 ℃ with 40 ℃ during design temperature, found, and saved bit by bit a large amount of gasoline in the receiving flask in second day.Subsequently, the inventor has carried out a large amount of tests, has found the method for dry gas system gasoline.
The economic benefit of dry gas system gasoline is considerable.As mentioned above, contain a considerable amount of ethene, propylene and butylene in the dry gas, by reacting the light Fuel oil product that can be translated into based on gasoline.Increase production 1.0 ten thousand tons of gasoline with the catalytic cracking unit of 1,000,000 tons of/year scales and estimate that as if 4000 yuan of increments per ton, then revenue growth is 40,000,000 yuan.Technology of the present invention is adopted in catalyzed cracking processing amount 100,000,000 tons of calculating in the whole nation, can increase income 4,000,000,000 yuan.
Literature survey shows, utilize the document and the patent of low-carbon alkene oligomerisation/superimposed production liquid many, " a kind of method with the hydrocarbon feed synthetic fluid hydrocarbon that contains C2～C6 alkene " disclosed as EP0439865A1, CN1155546C discloses " methods of low-carbon alkene oligomerisation or superimposed production carbon six above alkene ", CN1827564A discloses " a kind of method by the superimposed production diesel oil of C4 component that contains butylene ", CN1307133C discloses " a kind of building-up reactions method of low-carbon alkene ", CN1013347B discloses " the zeolite catalyst preparation method who is used for the superimposed production gasoline component of alkene low pressure ", or the like, in these patents or the document, low-carbon alkene mainly is the third rare and butylene, more at be butylene because the gas that contains propylene is isolated the third rare price far above the gas price by superimposed generation liquid by the gas branch.In all patents and document, still do not find to produce the bibliographical information of gasoline with catalysis drying gas.
Polymerization of low-carbon olefin is produced gasoline or diesel oil is thermopositive reaction, and catalyst system therefor mainly contains phosphoric acid salt and molecular sieve catalyst.Because the building-up reactions heat effect is very big, industrialization is very difficult.The present invention adopts special methods, and has adopted the structure-activity ingredient sieve catalyst of independent development, has overcome many practical difficulties.
Summary of the invention
The present invention utilizes the dry gas compositing characteristic, structure-activity ingredient sieve catalyst in conjunction with independent development, the heat effect of properly distributed reaction process, controlled polymerization degree or polymerisation run make in the dry gas 90% above olefinic polymerization generate light-weight fuel oil based on gasoline.Specific embodiment is as follows: dry gas is through heat exchange and/or be heated to 150～400 ℃, preferred 200～350 ℃, further preferred 250～300 ℃, enters bed from the fixed-bed reactor top through sparger.Bed can be divided into more than two sections or two sections to be loaded, the intersegmental interchanger of establishing, and then reach the purpose of controlling bed temperature.The bed service temperature is between 150～450 ℃, between preferred 250～400 ℃; Inject dry gas, gasoline or diesel oil since second section to bed, flow is decided on bed temperature.Reactor pressure is between 0.1～1.0MPa, between preferred 0.3～0.6MPa; The bed air speed is at 100～2000h
-1Between, preferred 300～1000h
-1Between.Oil, gas mixture flow out from reactor bottom and enter interchanger, enter gas-liquid separation tower or diesel oil absorption tower after the cooling, reclaim the gasoline that reaction generates.Dry gas behind the separation gasoline can be used as fuel gas, also can be used for other technological process.
The used catalyzer of the present invention is a molecular sieve catalyst, the preferred ZSM-5 of used molecular sieve, ZSM-11, HY, REY, USY molecular sieve a kind of, two or more, when using two or more mixed crystal molecular sieve, the acidity of catalyst center has obtained optimization.Most preferably be that the inventor invents, adopt in-situ crystallization method synthetic, have the ZIS molecular sieve of MFI structure.The Preparation of catalysts method is seen other patent.
Reactor of the present invention is the available stream fluidized bed reactor also, uses fluidized-bed can make temperature of reaction more even.When using fluidized-bed reactor, the dry gas of preheating injects from the bottom, flows out from the top.The dry gas preheating temperature is 100～400 ℃, preferred 150～300 ℃; Between fluidized-bed reaction pressure 0.1～1.0MPa, preferred 0.3～0.6Mpa; The fluidized-bed reaction temperature is between 200～450 ℃, between preferred 250～400 ℃; Volume space velocity is at 200～1500h
-1Between, preferred 300～800h
-1In the fluidized-bed reactor tubular heat exchanger can be set, also can adopt the dry gas sectional feeding.The used catalyzer of fluidized-bed reactor is the microballoon of 20～500um, and the microballoon of preferred 20～150um, this microballoon are in-situ crystallization ZIS molecular sieve catalysts, and this Preparation of catalysts method is seen another patent.
The present invention has following effect:
(1) dry gas olefin conversion height generally is higher than 85%, and under the situation of optimal conditions and catalyzer, olefin conversion is higher than 92%;
(2) yield of gasoline height, yield of gasoline accounts for more than 90% of olefin conversion;
(3) gasoline octane rating height, RON reaches more than 90;
(4) catalyst life is long, and in 3 months catalyzer one way life-spans, the repeated regeneration life-span reached more than 5 years.
Description of drawings
Below in conjunction with description of drawings method of the present invention.
Shown in the accompanying drawing 1, adopt fixed bed reactors, reaction oil gas directly obtains gasoline through heat exchange, condensation and gas-liquid separator. Raw material dry gas A and reacted high-temperature oil gas are carried out heat exchange in heat exchanger 3, then advance heating furnace 1 and be heated to uniform temperature, enter reactor from reactor head, and dry gas in the first paragraph beds exothermic reaction occurs; The cold raw material dry gas of another strand B injects from the top of second segment beds, behind the air-fuel mixture of cold dry gas and one section reaction, enters two sections beds and reacts. Total reaction oil gas flows out from the bottom of reactor, and through heat exchanger 3, condenser 4 enters gas-liquid separator 5, reclaims the gasoline that reaction generates, and the reaction dry gas flows out from the top of separator and enters pipe network or further processing.
Shown in the accompanying drawing 2, adopt fixed bed reactors, reaction oil gas is through heat exchange, condensation and diesel oil reabsorber, and gasoline enters in the absorption liquid, indirectly obtains gasoline through subsequent step. Raw material dry gas and reacted high-temperature oil gas are carried out heat exchange in heat exchanger 3, then advance heating furnace 1 and be heated to uniform temperature, divide two strands and enter reactor; One enters reactor from reactor head, in the first paragraph beds exothermic reaction occurs; Another strand injects from the top of second segment beds, behind the air-fuel mixture of this part dry gas and one section reaction, enters two sections beds and reacts. Total reaction oil gas flows out from the bottom of reactor, and through heat exchanger 3, condenser 4 enters diesel oil reabsorber 5, reclaims the gasoline that reaction generates, and the reaction dry gas flows out from cat head and enters pipe network or further processing, and gasoline enters absorption liquid.
Shown in the accompanying drawing 3, adopt fluidized-bed reactor, reaction oil gas directly obtains gasoline through heat exchange, condensation and gas-liquid separator. The raw material dry gas is divided into two strands, and one and reacted high-temperature oil gas are carried out heat exchange in heat exchanger 3, then advances heating furnace 1 and is heated to uniform temperature, enters from the fluidized-bed reactor bottom; The cold raw material dry gas of another strand injects from the position, middle and lower part of fluid bed. Total reaction oil gas flows out from the top of reactor, divides or filter is told solid catalyst through overwinding, and gas enters heat exchanger 3 successively, condenser 4, and gas-liquid separator 5 reclaims the gasoline that reaction generates, and the reaction dry gas enters pipe network or further processing.
Embodiment
Example 1
Certain refinery's heavy oil fluid catalytic cracking dry gas, composition sees Table 1.
Testing apparatus is the 100ml fixed-bed reactor.Dry gas is through the reducing valve control pressure, and the mass flowmeter dominant discharge enters in the fixed-bed reactor from top to down, and the oil gas that reaction generates by the variable valve control pressure, through condensation and gas-liquid separator, is told the gasoline that reaction generates through heat exchange.
The catalyzer that test is adopted is a kind of dry gas system gasoline catalyzing agent that the inventor develops, and the trade mark is DTG-1.Catalyzer is 3～4mm bead, piles than 0.91g/ml pore volume 0.27ml/g, specific surface 310m
2/ g.The catalyzer loading amount is 100ml, and the gas volume air speed is 500h
-1, 320 ℃ of preheating temperatures, 360 ℃ of bed temperatures, pressure 0.35MPa (gauge pressure) reacts and collected gasoline fraction 697.5g, olefin conversion 91% in 100 hours.The gasoline property that generates sees Table 2.
Table 1 dry gas is formed
| Dry gas is formed | Volume content, % | Mass content, % |
| Hydrogen | 31.19 | 3.64 |
| Methane | 28.3 | 26.44 |
| Ethane | 15.0 | 26.28 |
| Ethene | 12.0 | 19.62 |
| Propane | 0.5 | 1.28 |
| Propylene | 0.3 | 0.74 |
| Butane | 0.06 | 0.20 |
| Butylene | 0.05 | 0.16 |
| Carbon monoxide | 0.5 | 0.82 |
| Carbonic acid gas | 1.1 | 2.83 |
| Nitrogen | 11 | 17.99 |
The gasoline property that generates in table 2 example 1
| Title | Gasoline |
| Density (20 ℃), g.cm -3 | 0.7205 |
| Octane value RON | 90.3 |
| MON | 80.1 |
| Colloid, mg. (100mL) -1 | 0.11 |
| Sulphur content, μ g.g -1 | 60 |
| Nitrogen content, μ g.g -1 | 3 |
| Acidity, mgKOH. (100mL) -1 | 0.12 |
| Group composition, ω % | |
| Normal paraffin content, ω % | 5.7 |
| Isoparaffin content, ω % | 20.1 |
| Naphthene content, ω % | 15.3 |
| Olefin(e) centent, ω % | 22.2 |
| Aromaticity content, ω % | 36.7 |
| Boiling range, ℃ | |
| Fore-running | 36 |
| 10％ | 76 |
| 50％ | 118 |
| 90％ | 167 |
| Do | 185 |
Example 2
Conditions such as testing apparatus, raw material dry gas, catalyzer are with example 1, air speed 500h
-1, pressure 0.35MPa (gauge pressure) investigates the influence of temperature of reaction down.280 ℃, 320 ℃ and 400 ℃ of experiments, the oil-feed time all is 20h, and olefin conversion is respectively 80.2%, 90.1% and 96%, and quality of gasoline is respectively 123g, 137.5g and 126g.Transformation efficiency was low when temperature was low, but temperature is when reaching more than 320 ℃, and transformation efficiency all is higher than 90%.When temperature is higher than 400 ℃ and since the gasoline that generates again cracking cause oil to be received reducing.
Example 3
Other condition is identical, investigates the influence of gas space velocity.250h
-1, 500h
-1And 1000h
-1Three air speed experimental results are: olefin conversion is respectively 96.1%, 91% and 88.3%.
Example 4
Present embodiment carries out in fixed fluidized-bed reactor.Catalyzer is a microspherical catalyst, is a kind of in-situ crystallization ZIS molecular sieve catalyst.Dry gas is formed with example 1 (seeing Table 1).Catalyzer loading amount 200ml, 280 ℃ of dry gas preheating temperatures, the dry gas volume space velocity is 300h
-1, 380 ℃ of bed temperatures, pressure 0.25MPa (gauge pressure) reacts and collected gasoline fraction 86.7g, olefin conversion 95%, gasoline chromatography octane value RON91.2 in 10 hours.
Claims (11)
1, a kind of method of preparing gasoline with petroleum cracking of dry gas may further comprise the steps:
(1) dry gas preheating and/or be heated to certain temperature;
(2) dry gas enters beds from the fixed-bed reactor top; Under the effect of catalyzer, the part in the dry gas is formed the light-weight fuel oil that gasoline is rich in the generation that reacts, and oil, gas mixture flow out from reactor bottom together;
(3) enter gas-liquid separation tower or diesel oil absorption tower after oil, the gas mixture heat exchange cooling, reclaim the gasoline that reaction generates.
2,, it is characterized in that described petroleum cracking dry gas mainly refers to catalytic cracked dry gas, catalytic pyrolysis dry gas (DCC), coking dry gas etc. according to the method for claim 1; C in the dry gas feed composition
2 =And C
2 =Above alkene total mass percentage is in 5%～60% scope, and preferred range is 10～30%.
3, according to the method for claim 1, it is characterized in that in the step (1) that the raw material dry gas can and/or be heated to preheating temperature with reacted gas-oil mixture heat exchange, preheating temperature is 150～400 ℃, preferred 250～350 ℃.
4, according to the method for claim 1, it is characterized in that in the step (2) that the reaction conditions in the reactor is, between reaction pressure 0.1～1.0MPa, preferred 0.3～0.6Mpa; Temperature of reaction is between 200～500 ℃, between preferred 250～400 ℃; Volume space velocity is at 100～2000h
-1Between, preferred 300～1000h
-1
5,, it is characterized in that described beds can be divided into more than two sections or two sections, the intersegmental interchanger that is provided with according to the method for claim 1; Can feed a certain amount of dry gas, gasoline or diesel oil to every section since second section and regulate bed temperature.
6,, it is characterized in that in the described beds tubular heat exchanger being set according to the method for claim 1.
7, according to the method for claim 1, it is characterized in that it is molecular sieve that described activity of such catalysts structure is formed, this Preparation of catalysts method is seen another patent.
8, a kind of method of preparing gasoline with petroleum cracking of dry gas may further comprise the steps:
(1) dry gas preheating and/or be heated to certain temperature;
(2) dry gas enters beds from the fluidized-bed reactor bottom; Under the effect of catalyzer, the part in the dry gas is formed the light-weight fuel oil that gasoline is rich in the generation that reacts, and oil, gas mixture flow out from reactor head together;
(3) enter gas-liquid separation tower or diesel oil absorption tower after oil, the gas mixture heat exchange cooling, reclaim the gasoline that reaction generates.
9,, it is characterized in that described petroleum cracking dry gas mainly refers to catalytic cracked dry gas, catalytic pyrolysis dry gas (DCC), coking dry gas etc. according to the method for claim 8; C in the dry gas feed composition
2 =And C
2 =Above alkene total mass percentage is in 5%～60% scope, and preferred range is 10～30%.
10, according to the method for claim 8, it is characterized in that in the step (1) that the raw material dry gas can and/or be heated to preheating temperature with reacted gas-oil mixture heat exchange, preheating temperature is 100～400 ℃, preferred 150～300 ℃.
11, according to the method for claim 8, it is characterized in that in the step (2) that the reaction conditions in the reactor is, between reaction pressure 0.1～1.0MPa, preferred 0.3～0.6Mpa; Temperature of reaction is between 200～450 ℃, between preferred 250～400 ℃; Volume space velocity is at 200～1500h
-1Between, preferred 300～800h
-1
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101880546A (en) * | 2010-06-25 | 2010-11-10 | 山东齐旺达集团海仲化工科技有限公司 | Method for improving quality and reaction period in production of gasoline by using low-carbon hydrocarbons |
| CN102464547A (en) * | 2010-11-15 | 2012-05-23 | 上海河图石化工程有限公司 | Combined process for preparing propylene from liquefied gas and preparing petroleum from dry gas |
| CN102851063A (en) * | 2012-09-19 | 2013-01-02 | 北京惠尔三吉绿色化学科技有限公司 | Method for producing high-octane rating clean gasoline by dry gas and liquefied gas aromatization |
| CN109336726A (en) * | 2018-11-29 | 2019-02-15 | 北京惠尔三吉绿色化学科技有限公司 | A kind of technique of carbon four, light oil and coupling between methanol preparing propylene by catalytic cracking ethylene |
-
2008
- 2008-03-25 CN CNA2008100841266A patent/CN101343568A/en active Pending
Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101880546A (en) * | 2010-06-25 | 2010-11-10 | 山东齐旺达集团海仲化工科技有限公司 | Method for improving quality and reaction period in production of gasoline by using low-carbon hydrocarbons |
| CN101880546B (en) * | 2010-06-25 | 2013-12-25 | 山东齐旺达集团海仲化工科技有限公司 | Method for improving quality and reaction period in production of gasoline by using low-carbon hydrocarbons |
| CN102464547A (en) * | 2010-11-15 | 2012-05-23 | 上海河图石化工程有限公司 | Combined process for preparing propylene from liquefied gas and preparing petroleum from dry gas |
| CN102464547B (en) * | 2010-11-15 | 2014-12-10 | 上海河图工程股份有限公司 | Combined process for preparing propylene from liquefied gas and preparing petroleum from dry gas |
| CN102851063A (en) * | 2012-09-19 | 2013-01-02 | 北京惠尔三吉绿色化学科技有限公司 | Method for producing high-octane rating clean gasoline by dry gas and liquefied gas aromatization |
| CN102851063B (en) * | 2012-09-19 | 2014-10-22 | 北京惠尔三吉绿色化学科技有限公司 | Method for producing high-octane rating clean gasoline by dry gas and liquefied gas aromatization |
| CN109336726A (en) * | 2018-11-29 | 2019-02-15 | 北京惠尔三吉绿色化学科技有限公司 | A kind of technique of carbon four, light oil and coupling between methanol preparing propylene by catalytic cracking ethylene |
| CN109336726B (en) * | 2018-11-29 | 2024-05-31 | 北京惠尔三吉绿色化学科技有限公司 | Process for preparing propylene ethylene by coupling catalytic cracking of carbon four, light oil and methanol |
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