CN102399585B - Method for producing sweet gasoline - Google Patents
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- CN102399585B CN102399585B CN201010276690.5A CN201010276690A CN102399585B CN 102399585 B CN102399585 B CN 102399585B CN 201010276690 A CN201010276690 A CN 201010276690A CN 102399585 B CN102399585 B CN 102399585B
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Abstract
A method for producing sweet gasoline comprises the following steps of: (1) cutting a gasoline raw material into light gasoline fraction and heavy gasoline fraction, wherein the cut point of the light gasoline fraction and the heavy gasoline fraction is 50-100 DEG C; (2) carrying out non-hydrogenation desulfurization on the light gasoline fraction to obtain desulfurized light gasoline fraction; (3) under the hydrodesulfurization reaction condition, allowing the heavy gasoline fraction and hydrogen gas to contact with a hydrodesulfurization catalyst for selective hydrodesulfurization reaction to obtain desulfurized heavy gasoline fraction after separation; (4) mixing the desulfurized light gasoline fraction and the heavy gasoline fraction to obtain the gasoline product. When the heavy gasoline fraction and the hydrogen gas contact with the hydrodesulfurization catalyst in the step (3), a heavy distillate oil is also introduced to contact with the catalyst, wherein the initial boiling point of the heavy distillate oil is greater than the dry point of the gasoline distillate oil and the intake amount of the heavy distillate oil is 0.2h<-1>-2h<-1> when calculated according to liquid hourly space velocity.
Description
Technical field
The present invention relates to a kind of method of producing low-sulphur oil.
Background technology
Atmospheric pollution is a serious environmental problem, and the discharge of a large amount of engines is to cause one of air-polluting major reason.In recent years, be protection of the environment, countries in the world have proposed stricter restriction to the composition of motor spirit, to reduce the discharge of objectionable impurities.
At present, the sulphur of China's gasoline product has 90%～99% from catalytically cracked gasoline, and therefore, reducing sulfur content of catalytic cracking gasoline is the key point that reduces finished product content of sulfur in gasoline.
The sulphur content that reduces catalytically cracked gasoline can adopt catalytically cracked material to add hydrogen pretreatment (front-end hydrogenation) or two kinds of technical schemes of catalytic gasoline hydrogenation desulfurization (back end hydrogenation) conventionally.Wherein, catalytically cracked material pre-treatment can significantly reduce the sulphur content of catalytically cracked gasoline, but need to all under exacting terms, operate very much at temperature and pressure, simultaneously because unit capacity is large, cause hydrogen consumption also larger, these all will improve investment or the running cost of device.However, due to the heaviness of world's crude oil, increasing catalytic cracking unit starts to process the inferior raw material that contains normal, vacuum residuum etc., and therefore catalytically cracked material hydrogenation unit amount is also increasing year by year.Meanwhile, along with the innovation of catalytic cracking technology, catalytic cracking desulfurization auxiliary and/or fall the application gradually of alkene auxiliary agent, the sulfur content of catalytic cracking gasoline of China's Some Enterprises can reach below 500 μ g/g, or even below 150 μ g/g.But if further reduce the sulphur content of catalytically cracked gasoline, make it to be less than 50 μ g/g (meeting the restriction of Europe IV emission standard to content of sulfur in gasoline), even be less than 10 μ g/g (meeting the restriction of Europe V emission standard to content of sulfur in gasoline), just still need to set up again gasoline hydrogenation device.Compare front-end hydrogenation, catalytic gasoline hydrogenation desulfurization is all adding hydrogen pretreatment lower than catalytically cracked material aspect plant investment, production cost and hydrogen consumption.But adopt traditional catalyzer and technique, in hydrogenating desulfurization, the alkene significantly saturated meeting of hydrogenation causes product loss of octane number very large.One of effective way addressing the above problem is exactly to adopt selective hydrodesulfurization technology to process catalytically cracked gasoline.
US 6334948B1 has introduced a kind of low-sulphur oil production process, and that the first step first cuts into catalytic gasoline of whole fraction is light, weigh two kinds of cuts, and lighting end is used the catalyst based hydrogenating desulfurization of Ni; Selective hydrodesulfurization is carried out in last running, then light, last running after refining is mixed to get to full cut product.
CN 1224679C method of producing low-sulphur oil, by gasoline stocks be cut into gently, last running, wherein the cut point of light gasoline fraction and heavy naphtha is 80 DEG C～100 DEG C, lighting end is through soda finishing mercaptan removal, last running contacts with Hydrobon catalyst together with hydrogen, carry out selective hydrodesulfurization reaction, the gasoline fraction after hydrogenation carries out hydrogenation or non-hydro-sweetening, and light, last running after desulfurization are mixed to get to gasoline products.Olefin saturated rate is lower than 30% in the situation that gasoline desulfur rate is higher for the method, and the anti-knock index of gasoline loses lower than 2 units, and the gasoline products sulphur content of the method gained is greater than 50 μ g/g.
Summary of the invention
The technical problem to be solved in the present invention is to provide a kind of method newly, that desulfuration selectivity is better produced low-sulphur oil.
The invention provides a kind of method of producing low-sulphur oil, comprise the following steps:
(1), gasoline stocks is cut into light gasoline fraction, heavy naphtha, wherein, the cut point of light gasoline fraction and heavy naphtha is 50 DEG C～100 DEG C;
(2), light gasoline fraction is carried out to non-hydro-sweetening, obtain the light gasoline fraction after desulfurization;
(3), under gasoline hydrodesulfurizationmethod reaction conditions, heavy naphtha is contacted with Hydrobon catalyst together with hydrogen, carry out selective hydrodesulfurization reaction, be isolated to the heavy naphtha after desulfurization;
(4), the light gasoline fraction after desulfurization and heavy naphtha are mixed to get to gasoline products;
Wherein, in the time of step (3) described heavy naphtha is contacted with Hydrobon catalyst together with hydrogen, also comprise and introduce a kind of heavy distillate, the initial boiling point of described heavy distillate is greater than described gasoline fraction oil final boiling point, volume space velocity during in liquid, the introduction volume of heavy distillate is 0.2h
-1-2h
-1.
Wherein, described heavy distillate is selected from diesel oil distillate oil and/or lubricating oil distillate, and the temperature difference of the final boiling point of the initial boiling point of described heavy distillate and described gasoline fraction oil is not less than 1 DEG C, is preferably not less than 10 DEG C, further preferably be not less than 20 DEG C, be more preferably not less than 40 DEG C.Volume space velocity during in liquid, the introduction volume of heavy distillate is preferably 0.4h
-1-1.8h
-1, more preferably 0.6h
-1-1.8h
-1.Described heavy distillate is derived from for example, in oil, synthetic oil (: be selected from olefin oligomerization synthetic oil, Fischer-Tropsch synthesis oil and biosynthesizing oil) one or more.Under reaction conditions of the present invention, wherein said heavy distillate exists with the form of liquid at least partly.
Described gasoline hydrodesulfurizationmethod reaction conditions is usual gasoline hydrodesulfurizationmethod reaction conditions, and preferred operational condition comprises: volume space velocity 3h when reaction pressure 0.8MPa-3.2MPa, 200 DEG C-320 DEG C of temperature of reaction, gasoline fraction fluid
-1-8h
-1, hydrogen-oil ratio 200Nm
3/ m
3-600Nm
3/ m
3, further preferred reaction conditions comprises: volume space velocity 3h when reaction pressure 1MPa-2.4MPa, 220 DEG C-270 DEG C of temperature of reaction, gasoline fraction fluid
-1-6h
-1, hydrogen-oil ratio 300Nm
3/ m
3-500Nm
3/ m
3.
Ensureing that under the condition that is enough to described heavy distillate be introduced and contacted with catalyzer, the present invention does not limit the introducing method of described heavy distillate.For example, can be that first described heavy distillate is mixed with gasoline fraction oil, introduce afterwards reactor and contact with catalyzer under gasoline selective hydrodesulfurizationmodification reaction conditions; Also can be that described heavy distillate and gasoline fraction oil raw material are introduced respectively to reactor, under gasoline selective hydrodesulfurizationmodification reaction conditions, contact with catalyzer afterwards.
According to method provided by the present invention, wherein, described reactor can be any reactor that is suitable for gasoline fraction oil hydrogenation in prior art, for example fixed bed hydrogenation reactor.Described gasoline stocks can be one or more in catalytically cracked gasoline, catalytic cracking gasoline, straight-run spirit, coker gasoline, pyrolysis gasoline and pressure gasoline.The boiling range of described gasoline stocks is the usual boiling range of gasoline fraction oil, for example: be 30-220 DEG C.
The cut point of described light gasoline fraction and heavy naphtha is preferably 50-75 DEG C.In a preferred embodiment, be respectively the 30 heavy % in heavy %～60 and the heavy % in 40 heavy %～70 of gasoline stocks by cutting the yield of described light gasoline fraction and heavy naphtha.
According to method provided by the present invention, wherein, the method that described light gasoline fraction carries out non-hydro-sweetening can be any method except hydrogenating desulfurization in prior art.For example, can be to adopt the method that sorbent material adsorbs to carry out mercaptan removal, can be to adopt the method for alkali cleaning to carry out mercaptan removal.Carried out description about these methods 350 pages of " petroleum refining engineering " (volume two) (petroleum industry press, Lin Shixiong work, version in 1988), quoted as a reference here.
According to method provided by the present invention, wherein, the described separation of step (3) comprises any for obtaining the required separating step of object product, and described separation method and device are the usual method and apparatus adopting in this area.For example, adopt this area usual apparatus and method to carry out air lift to generating oil, to remove gaseous impuritieies such as generating the hydrogen sulfide that contains in oil, carry out afterwards the step of fractionation by distillation.The gasoline fraction oil being isolated to reclaims as product, and heavy distillate can partly or entirely recycle.
According to method provided by the present invention, wherein, described catalyzer can be any one or more Hydrobon catalyst that prior art provides.In a preferred embodiment, described catalyzer is the catalyzer of aluminum oxide or the carrier loaded VIB of silica-alumina and/or VIII family non-precious metal catalyst.In oxide compound and taking total catalyst weight as benchmark, catalyzer consists of: the heavy % in heavy %～30 of molybdenum and/or tungsten 5.0, and the heavy % in heavy %～5.0 of nickel and/or cobalt 0.5, and can contain or not contain a small amount of auxiliary agent that is selected from IA main group, IIA main group or VA subgroup.For example, at the disclosed Hydrobon catalyst of 200710099304.8,200710099302.9,200710099834.2 difference, all can be used as catalyzer for the present invention, be incorporated to the present invention here and quote.
According to method provided by the present invention, can also comprise afterwards a step of the heavy naphtha after hydrogenating desulfurization being carried out to hydro-sweetening or non-hydro-sweetening (as stripping or oxidation deodorizing method) in described step (3), further to reduce mercaptans content wherein.Described hydro-sweetening method is for being this area conventional method, and for example, in CN99107939.6, having provided a kind of petroleum fractions faces hydrogen/hydrofinishing process, quotes as a reference here.
In a concrete embodiment, the inventive method comprises the steps:
(1), gasoline stocks is cut into light gasoline fraction, heavy naphtha at 50 DEG C～100 DEG C, the yield of light gasoline fraction, heavy naphtha is respectively the 30 heavy % in heavy %～60, the 40 heavy % in heavy %～70 of gasoline stocks;
(2), light gasoline fraction is through the refining mercaptan removing wherein of alkali extracting;
(3), heavy naphtha contacts with Hydrobon catalyst together with hydrogen, carries out hydrodesulfurization reaction, separates hydrogenated oil and obtains lighter hydrocarbons and gasoline fraction, hydrogen-rich gas recycles;
(4), step (3) gained gasoline fraction is carried out to hydrogenation or non-hydro-sweetening;
(5), the heavy naphtha after desulfurization with refining after light gasoline fraction be mixed to get gasoline products;
Wherein, in the time of step (3) described heavy naphtha is contacted with Hydrobon catalyst together with hydrogen, also comprise and introduce a kind of heavy distillate, the initial boiling point of described heavy distillate is greater than described gasoline fraction oil final boiling point, volume space velocity during in liquid, the introduction volume of heavy distillate is 0.2h
-1-2h
-1.
Described heavy distillate is selected from diesel oil distillate oil and/or lubricating oil distillate, the temperature difference of the final boiling point of the initial boiling point of described heavy distillate and described gasoline fraction oil is not less than 1 DEG C, preferably be not less than 10 DEG C, be further preferably not less than 20 DEG C, be more preferably not less than 40 DEG C.The introduction volume of heavy distillate is preferably 0.4h
-1-1.8h
-1, more preferably 0.6h
-1-1.8h
-1.Described heavy distillate is derived from for example, in oil, synthetic oil (: be selected from olefin oligomerization synthetic oil, Fischer-Tropsch synthesis oil and biosynthesizing oil) one or more.The preferred reaction conditions of described step (3) comprises: volume space velocity 3h when reaction pressure 0.8MPa-3.2MPa, 200 DEG C-320 DEG C of temperature of reaction, gasoline fraction fluid
-1-8h
-1, hydrogen-oil ratio 200Nm
3/ m
3-600Nm
3/ m
3, further preferred reaction conditions comprises: volume space velocity 3h when reaction pressure 1MPa-2.4MPa, 220 DEG C-270 DEG C of temperature of reaction, gasoline fraction fluid
-1-6h
-1, hydrogen-oil ratio 300Nm
3/ m
3-500Nm
3/ m
3.
Compared with prior art, gasoline hydrodesulfurizationmethod of the present invention is active obviously to be improved, and has good hydrogenating desulfurization selectivity.
Embodiment
The following examples will be further described method provided by the invention, but not thereby limiting the invention.
Comparative example and embodiment Hydrobon catalyst used be numbered RSE-1, in oxide compound and taking total catalyst weight as benchmark, RSE-1 consists of: cobalt contents 2.3 % by weight, and molybdenum content 14.8 % by weight, it is prepared referring to Chinese patent 200710099834.2 embodiment 1.
Comparative example 1 illustrates in existing method, the effect that the heavy naphtha oil of gasoline fraction oil after cutting carries out hydrogenating desulfurization.
Comparative example 1
Taking RSE-1 as catalyzer, in fixed-bed reactor, a kind of catalytically cracked gasoline heavy distillate raw material A (cut point is 65 DEG C) is carried out to hydrogenating desulfurization.
The character of stock oil A is in table 1, and reaction product obtains gasoline fraction oil production through air lift, and the character of reaction conditions and product is listed in table 2.
Embodiment 1-4 explanation the invention provides in method, the effect that the heavy naphtha oil of gasoline fraction oil after cutting carries out hydrogenating desulfurization.
Embodiment 1
Adopt catalyzer, the reactor identical with comparative example 1, stock oil C is carried out to hydrogenating desulfurization.Stock oil C is the mixture of stock oil A and heavy distillate B (Fischer-Tropsch synthesis oil), and in mixture, the content of B is 30 volume %.Stock oil character is in table 1, and reaction product obtains gasoline fraction oil production and heavy distillate B through air lift, distillation, and the character of reaction conditions and product is listed in table 2.
Embodiment 2
Adopt catalyzer, the reactor identical with comparative example 1, stock oil E is carried out to hydrogenating desulfurization.Stock oil E is the mixture of stock oil A and heavy distillate D (white oil), and in mixture, the content of D is 30 volume %.Stock oil character is in table 1, and reaction product obtains gasoline fraction oil production and heavy distillate D through air lift, distillation, and the character of reaction conditions and product is listed in table 2.
Embodiment 3
Adopt catalyzer, the reactor identical with comparative example 1, stock oil G is carried out to hydrogenating desulfurization.Stock oil G is the mixture of stock oil A and heavy distillate F (VGO), and in mixture, the content of F is 15 volume %.Stock oil character is in table 1, and reaction product obtains gasoline fraction oil production and heavy distillate F through air lift, distillation, and the character of reaction conditions and product is listed in table 2.
Embodiment 4
Adopt catalyzer, the reactor identical with comparative example 1, stock oil I is carried out to hydrogenating desulfurization.Stock oil I is the mixture of stock oil A and heavy distillate H (No. 10 white oils), and in mixture, the content of H is 20 volume %.Stock oil character is in table 1, and reaction product obtains gasoline fraction oil production and heavy distillate H through air lift, distillation, and the character of reaction conditions and product is listed in table 2.
Table 1
Table 2
| Embodiment | Comparative example 1 | 1 | 2 | 3 | 4 |
| Processing condition | |||||
| Hydrogen dividing potential drop, MPa | 1.6 | 1.6 | 1.6 | 1.6 | 1.6 |
| Temperature of reaction, DEG C | 260 | 260 | 260 | 260 | 260 |
| Gasoline fraction liquid hourly space velocity, h -1 | 4 | 4 | 4 | 4 | 4 |
| Heavy distillate liquid hourly space velocity, h -1 | 0 | 1.7 | 1.7 | 0.7 | 1 |
| Hydrogen-oil ratio, Nm 3/m 3 | 400 | 400 | 400 | 400 | 400 |
| Product property | |||||
| Density (20 DEG C), g/cm 3 | 0.7758 | 0.801 | 0.812 | 0.801 | 0.7903 |
| Sulphur, μ g/g | 103 | 75.1 | 78.2 | 80.3 | 67.0 |
| Bromine valency, gBr/100ml | 20.6 | 22.7 | 23.3 | 22.6 | 23.4 |
| Desulfurization degree, % | 88.86 | 91.89 | 91.54 | 91.32 | 92.75 |
| Olefin saturated rate, % | 23.42 | 15.57 | 13.44 | 15.70 | 12.95 |
Claims (12)
1. a method of producing low-sulphur oil, comprises the following steps:
(1), gasoline fraction oil raw material is cut into light gasoline fraction, heavy naphtha, wherein, the cut point of light gasoline fraction and heavy naphtha is 50 DEG C～100 DEG C;
(2), light gasoline fraction is carried out to non-hydro-sweetening, obtain the light gasoline fraction after desulfurization;
(3), under gasoline hydrodesulfurizationmethod reaction conditions, heavy naphtha is contacted with Hydrobon catalyst together with hydrogen, carry out selective hydrodesulfurization reaction, be isolated to the heavy naphtha after desulfurization;
(4), the light gasoline fraction after desulfurization and heavy naphtha are mixed to get to gasoline products;
Wherein, in the time of step (3) described heavy naphtha is contacted with Hydrobon catalyst together with hydrogen, also comprise that introducing a kind of heavy distillate contacts with catalyzer, the initial boiling point of described heavy distillate is greater than described gasoline fraction oil final boiling point, volume space velocity during in liquid, the introduction volume of heavy distillate is 0.2h
-1-2h
-1, the heavy distillate being isolated to partly or entirely recycles; Described selective hydrodesulfurization reaction conditions comprises: volume space velocity 3h when pressure 0.8MPa～3.2MPa, 200 DEG C～320 DEG C of temperature, heavy naphtha liquid
-1～8h
-1, hydrogen-oil ratio 200Nm
3/ m
3～600Nm
3/ m
3, under described reaction conditions, wherein said heavy distillate exists with the form of liquid at least partly.
2. method according to claim 1, it is characterized in that, described heavy distillate is selected from diesel oil distillate oil and/or lubricating oil distillate, and the temperature difference of the final boiling point of the initial boiling point of described heavy distillate and described gasoline fraction oil is not less than 1 DEG C, and the introduction volume of heavy distillate is 0.4h
-1-1.8h
-1.
3. method according to claim 2, is characterized in that, the temperature difference of the final boiling point of the initial boiling point of described heavy distillate and described gasoline fraction oil is not less than 10 DEG C, and the introduction volume of heavy distillate is 0.6h
-1-1.8h
-1.
4. according to the method described in claim 1,2 or 3, it is characterized in that, the temperature difference of the final boiling point of the initial boiling point of described heavy distillate and described gasoline fraction oil is not less than 20 DEG C.
5. method according to claim 4, is characterized in that, the temperature difference of the final boiling point of the initial boiling point of described heavy distillate and described gasoline fraction oil is not less than 40 DEG C.
6. method according to claim 1 and 2, is characterized in that, described heavy distillate is derived from one or more in oil, synthetic oil.
7. method according to claim 6, is characterized in that, described synthetic oil is selected from olefin oligomerization synthetic oil, Fischer-Tropsch synthesis oil and biosynthesizing oil.
8. method according to claim 1, is characterized in that, one or more in described gasoline fraction grease separation catalytic cracking gasoline, catalytic cracking gasoline, straight-run spirit, coker gasoline, pyrolysis gasoline and pressure gasoline.
9. method according to claim 8, is characterized in that, the boiling range of described gasoline fraction oil is 30-220 DEG C.
10. method according to claim 1, is characterized in that, described selective hydrodesulfurization reaction conditions comprises: volume space velocity 3h when reaction pressure 1MPa-2.8MPa, 220 DEG C-270 DEG C of temperature of reaction, heavy naphtha liquid
-1-6h
-1, hydrogen-oil ratio 300Nm
3/ m
3-500Nm
3/ m
3.
11. methods according to claim 1, is characterized in that, described non-hydro-sweetening method is alkali wash.
12. methods according to claim 1, is characterized in that, also comprise afterwards a step of the heavy naphtha after hydrogenating desulfurization being carried out to hydro-sweetening or non-hydro-sweetening in described step (3).
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Families Citing this family (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103468311B (en) * | 2012-06-07 | 2015-08-26 | 中国石油化工股份有限公司 | A kind of method of producing low-sulphur oil |
| CN103773431B (en) * | 2012-10-24 | 2016-01-20 | 中国石油化工股份有限公司 | A kind of gasoline desulfating method |
| CN103773432B (en) * | 2012-10-24 | 2015-11-25 | 中国石油化工股份有限公司 | A kind of gasoline desulfating method |
| CN105670687A (en) * | 2016-01-13 | 2016-06-15 | 山东联星能源集团有限公司 | Catalytically cracked gasoline desulphurization method |
| CN112708461B (en) * | 2019-10-24 | 2022-06-24 | 中国石油化工股份有限公司 | Method for increasing yield of propylene and low-sulfur fuel oil components |
| CN112708460A (en) | 2019-10-24 | 2021-04-27 | 中国石油化工股份有限公司 | Process for producing low carbon olefins and low sulfur fuel oil components |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1465668A (en) * | 2002-06-27 | 2004-01-07 | 中国石油化工股份有限公司 | Method for producing low sulfur gasoline |
| CN101265417A (en) * | 2008-04-30 | 2008-09-17 | 山东金诚重油化工有限公司 | Method for providing heat for petroleum fractioning hydrogenation |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1465668A (en) * | 2002-06-27 | 2004-01-07 | 中国石油化工股份有限公司 | Method for producing low sulfur gasoline |
| CN101265417A (en) * | 2008-04-30 | 2008-09-17 | 山东金诚重油化工有限公司 | Method for providing heat for petroleum fractioning hydrogenation |
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