CN102634370A - Method for gasoline hydrogenation modification - Google Patents
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- CN102634370A CN102634370A CN201110035565XA CN201110035565A CN102634370A CN 102634370 A CN102634370 A CN 102634370A CN 201110035565X A CN201110035565X A CN 201110035565XA CN 201110035565 A CN201110035565 A CN 201110035565A CN 102634370 A CN102634370 A CN 102634370A
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Abstract
The invention relates to a method for gasoline hydrogenation modification; gasoline raw materials and hydrogen are mixed, and the mixture is allowed to enter a catalytic distillation tower for dialkene removal, and then to cut the gasoline into light and heavy components; light gasoline from the catalytic distillation tower top is directly used as a clean gasoline blending component; heavy gasoline from the bottom of the tower is allowed to enter a hydrogenation modification reactor for reactions such as aromatization, isomerization, and the like, and then to enter a hydrodesulfurization reactor for supplementary refining; materials from the hydrodesulfurization reactor is cooled, and is allowed to enter a product separation device for gas-liquid separation; hydrogen from the gas-liquid separation device is treated by desulphurization and then recycled; liquid products are allowed to enter a desulfurization tower for further reducing the mercaptan content of the gasoline, and then are mixed with the light gasoline to obtain the hydrogenation modified gasoline products; the method of the invention can not only greatly reduce sulfur and alkene contents in the gasoline, but also can reduce octane number loss due to the modification process.
Description
Technical field
The present invention relates to the method for secondary processing of gasoline hydro-upgradings such as a kind of hydrogenation modification method of inferior patrol, particularly catalytically cracked gasoline.
Background technology
In recent years, be the protection environment, countries in the world have proposed more strict restriction to the composition of motor spirit, to reduce emission of harmful substances.Beijing has carried out the provincial standard DB11/238-2007 of motor spirit Beijing on January 1st, 2008, and the standard code vehicle gasoline and sulfur content in vehicle gasoline is not more than 0.005% (m/m), and olefin(e) centent is not more than 30%.Estimate that Beijing will implement state V standard in 2012, the regulation vehicle gasoline and sulfur content in vehicle gasoline is not more than 0.001% (m/m), and olefin(e) centent is not more than 25%.The ratio of catalytically cracked gasoline has accounted for more than 80% in China's motor spirit, is alkene and sulfide main source in the gasoline.Therefore, the sulphur content that how to reduce catalytic gasoline is to improve the key of China's motor spirit quality.
The catalyzed gasoline hydrogenation desulfurization technology is main both at home and abroad at present divides two big types.One type is the selective hydrodesulfurization technology: through to catalyst modification, suppress the alkene saturated activity of catalyzer, in hydrogenating desulfurization, avoid alkene by too much saturated, reduce the loss of octane number of hydrogenation process.Another kind of technology is the catalytic gasoline modification technology: conventional hydrogenation catalyst is used in hydrogenating desulfurization; Through isomerizing, aromizing, cracking reaction hydrogenating desulfurization gasoline is handled then, the octane value that improves gasoline is to remedy the loss of octane number in the hydrodesulfurization process.
The ZL200410020932 patent discloses a kind of hydrogenation modification method of inferior patrol.This method is the process method that alkene falls in a kind of full cut FCC gasoline hydrodesulfurizationmethod.Under the condition that hydrogen exists and temperature raises gradually, contact with three kinds of catalyzer, form three reaction zones.First reaction zone temperature is lower, uses Hydrobon catalyst, mainly removes the diolefin in the gasoline; Second, third reaction zone temperature is high, and second reaction zone uses gasoline reforming catalyst, comprises the upgrading reaction of aromizing, isomerizing and benzene alkylation reaction, improves the octane value of gasoline, improves quality product; The 3rd reaction zone uses catalyst for selectively hydrodesulfurizing, removes organic sulfide in the oil to greatest extent.It is charging that this method adopts full cut catalytic gasoline, and loss of octane number is bigger.
The ZL200410060574 patent discloses a kind of inferior patrol hydrogenation modifying process.Its technological process is: feed gasoline is cut into lighting end and last running at 60～90 ℃; Wherein last running elder generation and hydrogen mix; Again with the Hydrobon catalyst contact reacts; Reacted elute contacts with the aromatization modification catalyzer and carries out the aromatization modification reaction, obtains high-octane rating low-sulphur oil cut; Heavy naphtha behind the upgrading mixes with lighting end or through the pretreated lighting end of mercaptan removal again, promptly gets product gasoline.This patent need adopt the method for sodafining mercaptan removal, can cause the discharging of the disagreeableness alkaline residue of environment.
The ZL200510090501 patent discloses a kind of method of gasoline hydrogenation modifying.Gasoline stocks is cut into light gasoline fraction and heavy naphtha, and light gasoline fraction removes mercaptan wherein through alkali cleaning refining desulfurization alcohol; The heavy gasoline cut contacts with catalyst for hydro-upgrading together with hydrogen and carries out hydrogenating desulfurization and hydro-upgrading reaction, and described catalyst for hydro-upgrading is a kind of catalyzer by zeolite and the carrier loaded non-noble metal components of aluminum oxide composite molding.This method is used a kind of catalyst for hydro-upgrading, and isomerizing, cracking, desulfurization, denitrogenation, alkene are saturated etc., and function is accomplished on same catalyzer.This patent also need adopt the method for sodafining mercaptan removal, can cause the discharging of the disagreeableness alkaline residue of environment.
The ZL200410102818 patent discloses a kind of gasoline modifying method.May further comprise the steps: a) under the isomerisation of olefin processing condition, gasoline fraction oil is contacted with the olefin skeletal isomerization catalyzer; B) under the hydrodesulfurization condition, the reaction effluent of step a) is contacted with Hydrobon catalyst.This method mainly adopts the method for isomerizing upgrading, and liquid product yield is lower.
US5411658 discloses a kind of method of gasoline upgrading, this method with catalytic gasoline unifining after, directly get into second section reactor drum and carry out octane value recovering.Traditional Hydrobon catalyst is adopted in this patent unifining, and loss of octane number is bigger.
Summary of the invention
The objective of the invention is to provide on the basis of existing technology a kind of method of inferior patrol hydro-upgrading.
Gasoline stocks mix with hydrogen at first get into a catalytic distillation tower remove diolefine and with gasoline cut into gently, two components of heavy petrol.The petroleum naphtha that comes out from the catalytic distillation column overhead is directly as the clean gasoline blend component, is introduced into a hydro-upgrading reactor drum after heavy petrol that comes out at the bottom of the tower and hydrogen mix, and then gets into a hydrodesulphurisatioreactors reactors and carry out post-refining.After the material cooling of coming out from hydrodesulphurisatioreactors reactors, get into product separator and carry out gas-liquid separation.The hydrogen that comes out from gas-liquid separator recycles after handling through desulfurization, and liquid-phase product gets into the mercaptan removal tower to be reduced after the mercaptans content in the gasoline to mix with petroleum naphtha and obtain the reformulated gasoline product.
The reaction conditions of above-mentioned catalytic distillation tower is: tower top pressure 0.5～2.0Mpa, 120～180 ℃ of feeding temperatures, 60～120 ℃ of tower top temperatures, 160～220 ℃ of column bottom temperatures, hydrogen to oil volume ratio 10～200.The support of the catalyst of catalytic distillation tower filling is the mixture of aluminum oxide, silicon oxide or aluminum oxide and silicon oxide; Reactive metal is selected from one or more among VIB or the VIIIB; MOX weight is 10%～70%; Specific surface area of catalyst is 100～300m2/g, and pore volume is 0.20～0.60ml/g.
The reaction conditions of above-mentioned hydro-upgrading reactor drum is: hydrogen dividing potential drop 1.0～4.0Mpa, 280～450 ℃ of temperature of reaction, volume space velocity 1.0～4.0h
-1, hydrogen to oil volume ratio 100～600.The catalyst for hydro-upgrading carrier is ZSM-5, Beta, SAPO molecular sieve or its mixture; By catalyst weight 100%, molecular sieve weight is 60%～90%, and MOX weight is 1%～10%; Reactive metal is selected from one or more among VIB or the VIIIB, and surplus is a sticker.Specific surface area of catalyst is 200～500m
2/ g, pore volume are 0.20～0.50ml/g.
The reaction conditions of above-mentioned hydrodesulphurisatioreactors reactors is: hydrogen dividing potential drop 1.0～4.0Mpa, 200～350 ℃ of temperature of reaction, volume space velocity 2.0～8.0h
-1, hydrogen to oil volume ratio 100～600.Hydrodesulfurization catalyst support is the mixture of aluminum oxide, silicon oxide or aluminum oxide and silicon oxide; Reactive metal is selected from one or more among VIB or the VIIIB; By catalyst weight 100%, MOX weight is 10%～30%, and specific surface area of catalyst is 100～300m
2/ g, pore volume are 0.20～0.80ml/g.
The reaction conditions of above-mentioned mercaptan removal tower is: hydrogen dividing potential drop 0.5～2.0Mpa, feeding temperature 200-300 ℃, tower top temperature 180-280 ℃, column bottom temperature 250-350 ℃, hydrogen to oil volume ratio 5～50.Mercaptan-eliminating catalyst is aluminum oxide, silicon oxide or its mixture or without hydrogen exchange na-pretreated zeolite.
Gasoline hydrogenation modifying process provided by the invention mainly contains following advantage:
1, the flow process of the present invention's employing; Not only reduced olefin content in gasoline; Also significantly reduce the mercaptans content in the gasoline, substituted sodafining mercaptan removal operation among patent ZL200410060574, the ZL200510090501, avoided the discharging of the disagreeableness alkaline residue of environment.
2, the present invention mainly adopts the aromatization modification technology, the isomerizing modification technology that relative patent ZL200410102818 adopts, and loss of octane number is little, and liquid is received high.
3, the present invention has adopted the flow process of first upgrading back end hydrogenation, and with respect to the flow process of upgrading behind the first hydrogenation of employings such as patent ZL200410060574, product aromizing rate is high, and loss of octane number is little.
4, the refining catalyst for selectively hydrodesulfurizing that adopts behind the present invention, for the Hydrobon catalyst that patent ZL200510090501, US5411658 use, the loss of octane number that hydrogenation process is brought is littler.
Description of drawings
Fig. 1 is the principle flow chart of gasoline hydrogenation modifying method provided by the present invention.
Embodiment
Technical process of the present invention is: gasoline stocks and hydrogen are mixed catalytic distillation tower of back entering; Under tower top pressure 0.5～2.0Mpa, 120～180 ℃ of feeding temperatures, 60～120 ℃ of tower top temperatures, 160～220 ℃ of column bottom temperatures, hydrogen to oil volume ratio 10～200 conditions, carry out hydrogenation reaction, with the diene in the catalytic gasoline saturated and with gasoline be divided into light, weigh two components.Heavy petrol mixes the back and gets into the hydro-upgrading reactor drum with hydrogen, at hydrogen dividing potential drop 1.0～4.0Mpa, 280～450 ℃ of temperature of reaction, volume space velocity 1.0～4.0h
-1, under hydrogen to oil volume ratio 100～500 conditions, aromizing, isomerization reaction take place, follow reactions such as desulfurization, alkene be saturated simultaneously.Through hydro-upgrading, olefin content in gasoline, sulphur content reduce significantly.The hydro-upgrading reaction product gets into hydrodesulphurisatioreactors reactors then and carries out post-refining, at hydrogen dividing potential drop 1.0～4.0Mpa, 200～350 ℃ of temperature of reaction, volume space velocity 2.0～8.0h
-1, under hydrogen to oil volume ratio 100～500 conditions, further reduce olefin content in gasoline and sulfide content.After the cooling of hydrogenating desulfurization product, get into product separator separation carrying out gas-liquid separation.The hydrogen that comes out from gas-liquid separator recycles after handling through desulfurization; Liquid-phase product gets into the mercaptan removal tower, after hydrogen dividing potential drop 0.5～2.0Mpa, feeding temperature 200-300 ℃, tower top temperature 180-280 ℃, column bottom temperature 250-350 ℃ reaction conditions remove the mercaptan in the gasoline earlier, mixes and obtains the reformulated gasoline product with the fractionator overhead petroleum naphtha that comes out.
The present invention is applicable to the hydro-upgrading of inferior patrol, is mainly used in the hydro-upgrading of secondary processing of gasoline such as catalytically cracked gasoline, catalytic cracking gasoline, coker gasoline and pressure gasoline.
Gasoline upgrading technology of the present invention is characterized in that adopting full distillation gasoline pre-treatment, and light then, heavy petrol separates, and heavy petrol adopts the technical process of first hydro-upgrading back end hydrogenation desulfurization.
Comparative Examples
With a kind of catalytically cracked gasoline is raw material, and its character is as shown in table 1.Catalytic gasoline at first gets into catalytic distillation tower, under tower top pressure 0.75Mpa, 145 ℃ of feeding temperatures, 90 ℃ of tower top temperatures, 205 ℃ of conditions of column bottom temperature, reacts, and is cut into two components of weight gasoline simultaneously, and heavy naphtha accounts for 65% of raw material.Heavy petrol at first is mixed into hydrodesulphurisatioreactors reactors with hydrogen, under hydrogen dividing potential drop 1.8MPa, 252 ℃ of conditions, carries out hydrogenating desulfurization.Get into the hydro-upgrading reactor drum then and under the reaction conditions of 385 ℃ of hydrogen dividing potential drop 2.0MPa, temperature of reaction, carry out hydro-upgrading.The hydro-upgrading product mixes with petroleum naphtha after stabilizer tower is stable and obtains the clean gasoline product.Processing condition are seen table 2 with generation oiliness matter.Can find out that from table 2 the product sulphur content is 66ppm, desulfurization degree 81.5%, olefin(e) centent drops to 27.8%, 1.1 units of octane value (RON) loss from 48.5%.
Embodiment 1
The raw oil that embodiment 1 uses is identical with Comparative Examples.Catalytic gasoline at first gets into catalytic distillation tower, under tower top pressure 0.75Mpa, 145 ℃ of feeding temperatures, 90 ℃ of tower top temperatures, 205 ℃ of conditions of column bottom temperature, reacts, and is cut into two components of weight gasoline simultaneously, and heavy naphtha accounts for 65% of raw material.Heavy petrol at first is mixed into the hydro-upgrading reactor drum with hydrogen, under the reaction conditions of 385 ℃ of hydrogen dividing potential drop 2.0MPa, temperature of reaction, carries out hydro-upgrading, gets into hydrodesulphurisatioreactors reactors then and under hydrogen dividing potential drop 1.8MPa, 252 ℃ of conditions, carries out hydrogenating desulfurization.Product gets into the mercaptan removal tower then after the desulfurization, after the mercaptans content that further reduces gasoline under hydrogen dividing potential drop 1.8Mpa, 300 ℃ of feeding temperatures, 260 ℃ of tower top temperatures, 350 ℃ of column bottom temperatures, hydrogen to oil volume ratio 50 conditions, mixes and obtains the reformulated gasoline product with the fractionator overhead petroleum naphtha that comes out.Processing condition are seen table 2 with generation oiliness matter.Can find out that from table 2 the product sulphur content is 45ppm, desulfurization degree 87.4%, olefin(e) centent drops to 29.5%, 0.5 unit of octane value (RON) loss from 48.5%.
Embodiment 2
The raw oil that embodiment 2 uses is identical with Comparative Examples.Catalytic gasoline at first gets into catalytic distillation tower and under tower top pressure 0.75Mpa, 145 ℃ of feeding temperatures, 90 ℃ of tower top temperatures, 205 ℃ of conditions of column bottom temperature, reacts, and is cut into two components of weight gasoline simultaneously, and heavy naphtha accounts for 65% of raw material.Heavy petrol at first is mixed into the hydro-upgrading reactor drum with hydrogen, under the reaction conditions of 385 ℃ of hydrogen dividing potential drop 2.0MPa, temperature of reaction, carries out hydro-upgrading, gets into hydrodesulphurisatioreactors reactors then and under hydrogen dividing potential drop 1.8MPa, 265 ℃ of conditions, carries out hydrogenating desulfurization.Product gets into the mercaptan removal tower after the desulfurization, after the mercaptans content that further reduces gasoline under hydrogen dividing potential drop 1.8Mpa, 300 ℃ of feeding temperatures, 260 ℃ of tower top temperatures, 350 ℃ of column bottom temperatures, hydrogen to oil volume ratio 50 conditions, mixes and obtains the reformulated gasoline product with the fractionator overhead petroleum naphtha that comes out.Processing condition are seen table 2 with generation oiliness matter.Can find out that from table 2 sulphur content is 20ppm in the product, desulfurization degree 94.4%, olefin(e) centent drops to 28.1%, 1.1 units of octane value (RON) loss from 48.5%.
Table 1
| Material name | Catalytic gasoline |
| Density (20 ℃), g/cm 3 | 0.721 |
| Sulphur, ppm | 356 |
| Olefin(e) centent, volume % | 48.5 |
| Boiling range, ℃ | |
| Over point | 36 |
| 10％ | 52 |
| 50％ | 96 |
| Do | 197 |
| Octane value (RON) | 92 |
Table 2
| Comparative Examples 1 | Embodiment 1 | Embodiment 2 | |
| Processing condition | |||
| The catalytic distillation tower tower top pressure, MPa | 0.75 | 0.75 | 0.75 |
| The catalytic distillation tower feeding temperature, ℃ | 145 | 145 | 145 |
| The catalytic distillation tower tower top temperature, ℃ | 90 | 90 | 90 |
| The catalytic distillation tower column bottom temperature, ℃ | 205 | 205 | 205 |
| Preparatory hydrogenation temperature, ℃ | 160 | 160 | 90 |
| Hydro-upgrading pressure, MPa | 2.0 | 2.0 | 205 |
| The hydro-upgrading temperature, ℃ | 385 | 385 | 385 |
| Hydrogenating desulfurization pressure, MPa | 1.8 | 1.8 | 1.8 |
| The hydrogenating desulfurization temperature, ℃ | 252 | 252 | 265 |
| Mercaptan removal column overhead pressure, MPa | 1.8 | 1.8 | |
| Mercaptan removal tower feeding temperature, ℃ | 300 | 300 | |
| Mercaptan removal column overhead temperature, ℃ | 260 | 260 | |
| Temperature at the bottom of the mercaptan removal Tata, ℃ | 350 | 350 | |
| Product property | |||
| Density, (20 ℃), g/cm 3 | 0.713 | 0.715 | 0.712 |
| Sulphur content, ppm | 66 | 45 | 20 |
| Olefin(e) centent, volume % | 27.8 | 29.5 | 28.1 |
| Octane value (RON) | 90.9 | 91.5 | 90.9 |
| Loss of octane number | 1.1 | 0.5 | 1.1 |
| Desulfurization degree % | 81.5 | 87.4 | 94.4 |
Claims (2)
1. the method for a gasoline hydrogenation modifying is characterized in that:
(1) earlier with gasoline stocks and hydrogen be mixed into catalytic distillation tower remove diolefine and with gasoline cut into gently, two components of heavy petrol; Reaction conditions is: tower top pressure 0.5～2.0Mpa, 120～180 ℃ of feeding temperatures, 60～120 ℃ of tower top temperatures, 160～220 ℃ of column bottom temperatures, hydrogen to oil volume ratio 10～200; Support of the catalyst is the mixture of aluminum oxide, silicon oxide or aluminum oxide and silicon oxide, and reactive metal is selected from one or more among VIB, the VIIIB, and by catalyzer 100%, MOX weight is 10～70%, and surplus is a carrier; Specific surface area of catalyst is 100～300m
2/ g, pore volume are 0.20～0.60ml/g
(2) petroleum naphtha that comes out from the catalytic distillation column overhead is directly as the clean gasoline blend component;
(3) heavy petrol that comes out at the bottom of the tower and hydrogen are introduced into the hydro-upgrading reactor drum after mixing; Reaction conditions is: hydrogen dividing potential drop 1.0～4.0Mpa, 280～450 ℃ of temperature of reaction, volume space velocity 1.0～4.0h
-1, hydrogen to oil volume ratio 100～600; Support of the catalyst is ZSM-5, Beta, SAPO molecular sieve or its mixture; By catalyzer 100%, molecular sieve weight is 60～90%, and MOX weight is 1～10%; Reactive metal is selected from one or more among VIB, the VIIIB, and surplus is a sticker; Specific surface area of catalyst is 200～500m
2/ g, pore volume are 0.20～0.50ml/g;
(4) get into hydrodesulphurisatioreactors reactors then and carry out post-refining; Reaction conditions is: hydrogen dividing potential drop 1.0～4.0Mpa, 200～350 ℃ of temperature of reaction, volume space velocity 2.0～8.0h
-1, hydrogen to oil volume ratio 100～600; Support of the catalyst is the mixture of aluminum oxide, silicon oxide or aluminum oxide and silicon oxide, and reactive metal is selected from one or more among VIB, the VIIIB, and by catalyst weight 100%, metal oxide content is 10～30%, and surplus is a carrier; Specific surface area of catalyst is 100～300m
2/ g, pore volume are 0.20～0.80ml/g;
(5) after the material that comes out from hydrodesulphurisatioreactors reactors cools off, get into product separator and carry out gas-liquid separation;
(6) after handling through desulfurization, the hydrogen that comes out from gas-liquid separator recycles;
(7) liquid-phase product gets into the mercaptan removal tower and further reduces after the mercaptans content in the gasoline to mix with petroleum naphtha and obtain the reformulated gasoline product; Reaction conditions is: hydrogen dividing potential drop 0.5～2.0Mpa, feeding temperature 200-300 ℃, tower top temperature 180-280 ℃, column bottom temperature 250-350 ℃, hydrogen to oil volume ratio 5～50; Catalyzer is aluminum oxide, silicon oxide or its mixture or without hydrogen exchange na-pretreated zeolite.
2. according to the described method of claim 1, it is characterized in that described gasoline stocks is one or more the mixing oil in catalytically cracked gasoline, catalytic cracking gasoline, coker gasoline and the pressure gasoline.
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| WO2018072342A1 (en) * | 2016-10-21 | 2018-04-26 | 中国石油化工股份有限公司 | Petrol treatment method |
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