CN102199448A - Process method for reducing olefins by hydrogen desulfurization of catalytic gasoline - Google Patents
Process method for reducing olefins by hydrogen desulfurization of catalytic gasoline Download PDFInfo
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- CN102199448A CN102199448A CN2010101347459A CN201010134745A CN102199448A CN 102199448 A CN102199448 A CN 102199448A CN 2010101347459 A CN2010101347459 A CN 2010101347459A CN 201010134745 A CN201010134745 A CN 201010134745A CN 102199448 A CN102199448 A CN 102199448A
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Abstract
The invention relates to a process method for reducing olefins by the hydrogen desulfurization of catalytic gasoline, which comprises the following steps of: cutting gasoline into a light distillate and a heavy distillate at the cutting point of between 60 and 80 DEG C; contacting the heavy distillate and hydrogen with an octane value restoration catalyst to perform an isomerization reaction, an aromatization reaction and a building-up reaction; and contacting reaction effluents which are not separated with a selective hydrogen desulfurization catalyst to perform a hydrogen desulfurization reaction, and separating hydrogenated generation oil to obtain light hydrocarbons and gasoline distillates, wherein hydrogen-enriched gas is recycled, the octane value restoration catalyst is used for loading one or two VIB or VIII group metal as active ingredients by taking one or more of aluminum oxides or molecular sieves as a carrier, an aid is one or two oxides in IIB groups or lanthanide series, the selective hydrogen desulfurization catalyst takes the aluminum oxides as the carrier, Mo and Co as active metal and one or more of Ce, Mg, K, P and F as the aid, the olefin content is less than 20 volume percent, the sulfur content is less than 50 micrograms/gram, and research octane number (RON) is improved by 1.5 to 2 units.
Description
Technical field
The present invention relates to the method for secondary processing whole-distillate gasoline hydro-upgradings such as a kind of processing method of catalytic gasoline hydrogenation desulfurating and reducing olefinic hydrocarbon, particularly FCC.
Background technology
The sulphur content and the olefin(e) centent of gasoline products all have certain restriction at present.Sulphur and olefin(e) centent are all higher in the secondary processing of gasoline such as FCC, and therefore, sulphur content and olefin(e) centent are the keys that solves the FCC quality of gasoline in the secondary processing of gasoline such as reduction FCC.
Adopt traditional hydrofining technology to carry out the FCC gasoline desulfur, fall alkene, the loss of octane number of product is bigger, and RON can lose 7～10 units, has also increased the hydrogen consumption simultaneously; Adopt the selective hydrodesulfurization method, sulphur content can be taken off to very low, but alkene reduction amplitude is little; Adopt the method for independent gasoline upgrading, though can reduce the loss of RON by isomerization, aromizing and building-up reactions, the amplitude that sulphur content reduces is limited, and particularly it does rise behind the gasoline upgrading, influences yield of gasoline.
The give chapter and verse difference of gasoline boiling point of US4131517 becomes several fractions with gasoline rectifying, three kinds of fractions preferably, and then under different condition, carry out desulfurization respectively.Above-mentioned technology can be by than the caustic wash desulfuration and the heavy fraction hydrogenating desulfurization of light fraction, and the purpose of reach and fall alkene, falling sulphur can avoid again that light olefin is saturated to cause too much loss of octane number.Above-mentioned technology exists significantly not enough, and it is limited that is exactly the amplitude that reduces of alkene.Reduce more for a long time at product requirement alkene, can not avoid the too much loss of octane value.
The disclosed gasoline modifying method of US5411658 is that elder generation adopts beta-zeolite catalyst that the effluent of hydrofining reaction is carried out octane value recovering after adopting traditional Hydrobon catalyst with the FCC gasoline hydrofinishing again.But this method uses the raw material final boiling point higher, and the too high aromatic hydrocarbons that makes of hydrofining section temperature of reaction is saturated too much, causes the RON loss more, is difficult to recover.
The disclosed a kind of inferior patrol hydrogenation modifying process of CN1621495A is that feed gasoline is cut into light fraction and heavy fraction at 60～90 ℃, heavy fraction mixes with hydrogen, again with the Hydrobon catalyst contact reacts, reaction effluent contacts with the aromatization modification catalyzer and carries out aromatization modification reaction, is 150ppm but the content of sulfur in gasoline that uses the described catalyzer of this method to obtain is still very high.
The method of the disclosed deep desulfurization olefin hydrocarbon reduction of gasoline of CN1465666A be with gasoline stocks be cut into gently, heavy fraction, heavy fraction contacts with octane value recovering catalyst with Hydrobon catalyst successively, light, heavy fraction after the desulfurization is mixed obtaining gasoline products.The content of sulfur in gasoline that this method is produced drops to 200ppm, and yield of gasoline is undesirable.
The method for modifying of disclosed gasoline of US5599439 and reformed oil is, first section is carried out hydrofining earlier, it is saturated to deviate from impurity such as sulphur, nitrogen and alkene, pass through again intermediate section from, the gas that process is isolated behind the impurity such as hydrogen sulfide, ammonia directly loops back first section, intermediates oil enters second section, carries out the octane value recovering process in fluidized-bed reactor, and this section is not being mended new hydrogen.This method has increased a separator between one, two section, increase facility investment, and working pressure is low excessively simultaneously, is unfavorable for the long-term operation of catalyzer.
Summary of the invention
The processing method of alkene falls in the gasoline hydrodesulfurizationmethod that the objective of the invention is advantages such as providing a kind of liquid receipts height on the basis of existing technology, the hydrogen consumption is low, octane value increases.
The processing method of a kind of catalytic gasoline hydrogenation desulfurating and reducing olefinic hydrocarbon of the present invention comprises the following steps:
(1) whole-distillate gasoline is cut into light, weigh two fractions, cut point is 60～80 ℃, the cutting principle thiophene is cut in the heavy fraction;
(2) light fraction removes wherein mercaptan through alkali cleaning refining desulfurization alcohol;
(3) heavy fraction contacts with octane value recovering catalyst earlier with hydrogen, carries out isomerization, aromizing and building-up reactions;
(4) reaction effluent contacts with catalyst for selectively hydrodesulfurizing without separation again, carries out hydrodesulfurization reaction, separates hydrogenated oil and obtains lighter hydrocarbons and gasoline fraction, and hydrogen-rich gas recycles;
(5) the heavy petrol fraction behind the hydro-upgrading with refining after the petroleum naphtha fraction mix and obtain gasoline products;
Wherein the described reaction conditions of step (3) is hydrogen dividing potential drop 1.5～3.0MPa, 360～430 ℃ of temperature of reaction, volume space velocity 1.2～3.0h-1, hydrogen to oil volume ratio 200～600, and catalyzer is the gasoline octane rating restorative;
The described reaction conditions of step (4) is hydrogen dividing potential drop 1.5～3.0MPa, 240～320 ℃ of temperature of reaction, volume space velocity 2.4～6.0h-1, hydrogen to oil volume ratio 200～600, and catalyzer is the gasoline selective hydrodesulfurizationmodification restorative;
The whole-distillate gasoline gasoline stocks is catalytically cracked gasoline, coker gasoline, pyrolysis gasoline, pressure gasoline or its mixture;
Described octane value recovering catalyst is the commercially available trade names FO-3558 of Fushun Petrochemical Company, with in aluminum oxide or the molecular sieve one or more is carrier, one or both VIB of load or VIII family metal are active ingredient, auxiliary agent is one or both oxide compounds in IIB family or the group of the lanthanides, by catalyst weight per-cent: active ingredient is 5～25%, auxiliary agent is 1～10%, and carrier is 74～94%;
Described catalyst for selectively hydrodesulfurizing is the commercially available trade names FF-21 of Fushun Petrochemical Company, is carrier with the aluminum oxide, and Mo and Co are reactive metal, and one or more among Ce, Mg, K, P, the F are auxiliary agent, by catalyst weight per-cent: MoO
3Be 7.0～18.0%, CoO is 1.0～6.0%, auxiliary agent is 0.2～10.2%, all the other are the carrier amount;
Step (3) and step (4) are carried out in a reactor, or carry out in two reactors; When using a reactor, octane value recovering catalyst is seated in the reactor epimere, and catalyst for selectively hydrodesulfurizing is seated in the reactor hypomere.
Compared with prior art, the present invention has the following advantages:
(1) alkene, the higher inferior full fraction FCC gasoline of sulphur content can be processed as the premium product.As can with the olefin(e) centent of full fraction FCC gasoline and sulphur content respectively by be reduced to olefin(e) centent＜20v% about 45v%, 500 μ g/g, sulphur content＜50 μ g/g, RON improves 1.5～2 units.
(2) heavy fraction gasoline contact with octane value recovering catalyst earlier, and is higher owing to olefin(e) centent, and it is bigger to carry out isomerization, aromizing and building-up reactions amplitude, and the octane value raising is also big; Contact with the selective hydrodesulfurization agent, carry out hydrodesulfurization reaction, alkene can be further saturated, but saturated amplitude is less, and sulphur content reduces significantly.Therefore, when content of sulfur in gasoline, alkene reduced significantly, octane value can be improved.
(3) cut point that the full fraction of gasoline is cut into petroleum naphtha fraction and heavy petrol fraction is 60～80 ℃, and the fractionation principle is that thiophene does not enter the petroleum naphtha fraction, because the alkali cleaning of petroleum naphtha fraction is refining when removing mercaptan, thiophene does not react.
(4) technology is simple, stable operation.Can adopt serial flow, the centre does not need separating device.
Description of drawings
Fig. 1 is the Technology synoptic diagram that alkene falls in gasoline hydrodesulfurizationmethod provided by the invention.
Embodiment
The method that present technique provides is so concrete enforcement:
(1) whole-distillate gasoline is cut into light, weigh two fractions, cut point is 60～80 ℃, the cutting principle thiophene is cut in the heavy fraction;
(2) light fraction removes wherein mercaptan through alkali cleaning refining desulfurization alcohol;
(3) heavy fraction contacts with octane value recovering catalyst earlier with hydrogen, carries out isomerization, aromizing and building-up reactions;
(4) reaction effluent contacts with catalyst for selectively hydrodesulfurizing without separation again, carries out hydrodesulfurization reaction, separates hydrogenated oil and obtains lighter hydrocarbons and gasoline fraction, and hydrogen-rich gas recycles;
(5) the heavy petrol fraction behind the hydro-upgrading with refining after the petroleum naphtha fraction mix and obtain gasoline products.
Used alkali is sodium hydroxide solution etc. in the step (2).
The described reaction conditions of step (3) is hydrogen dividing potential drop 1.5～3.0MPa, 360～430 ℃ of temperature of reaction, volume space velocity 1.2～3.0h-1, hydrogen to oil volume ratio 200～600, and catalyzer is the gasoline octane rating restorative.Catalyzer is the commercially available trade names FO-3558 of Fushun Petrochemical Company, to load on one or more complex carriers in aluminum oxide or the molecular sieve, the content of catalyzer is by weight percentage: active component content is 5～25%, is one or both VIB or VIII family metal; Auxiliary agent content is 1～10%, is one or both oxide compounds in IIB family or the group of the lanthanides; Vector contg is 74～94%.
The described reaction conditions of step (4) is hydrogen dividing potential drop 1.5～3.0MPa, 240～320 ℃ of temperature of reaction, volume space velocity 2.4～6.0h
-1, hydrogen to oil volume ratio 200～600, catalyzer is the gasoline selective hydrodesulfurizationmodification agent.Catalyzer is the commercially available trade names FF-21 of Fushun Petrochemical Company, is carrier with the aluminum oxide, and Mo and Co are reactive metal, and one or more among Ce, Mg, K, P, the F are auxiliary agent, and wherein catalyzer contains MoO
37.0～18.0w%, CoO1.0～6.0w%, auxiliary agent 0.2～10.2w%.
Step (3) and step (4) are carried out in a reactor, or carry out in two reactors; When using a reactor, octane value recovering catalyst is seated in the reactor epimere, and catalyst for selectively hydrodesulfurizing is seated in the reactor hypomere.
Below in conjunction with accompanying drawing to technology further instruction provided by the present invention.But it is not thereby limiting the invention.
Accompanying drawing is the Technology synoptic diagram that alkene falls in gasoline hydrodesulfurizationmethod provided by the invention.
The flow process of this technology is as follows:
Gasoline stocks enters through pipeline 1 that separation column 2 is cut into gently, the heavy petrol fraction, and wherein, the petroleum naphtha fraction enters alkali cleaning unit 5 through pipeline 3, and the petroleum naphtha fraction after the alkali cleaning is drawn through pipeline 6; The heavy petrol fraction enters pump 7 through pipeline 4, through pipeline 8 with after hydrogen-rich gas from pipeline 22 mixes, entering fixed-bed reactor 12 through pipeline 9, interchanger 10, pipeline 11 successively contacts with the octane value recovering agent, reaction effluent enters fixed bed desulphurization reactor 14 through pipeline 13, contacts with catalyst for selectively hydrodesulfurizing.The reaction effluent of reactor 14 enters high score 17 through pipeline 15, interchanger 10, pipeline 16 successively, the hydrogen-rich gas that comes out from high score 17 tops is through depriving hydrogen sulphide jar 28, enter compressor 19 by pipeline 18, hydrogen-rich gas after the compression through pipeline 20 or with from the fresh hydrogen of pipeline 21 through pipeline 22, and enter fixed-bed reactor 12 through pipeline 9, interchanger 10, pipeline 11 successively after heavy petrol fraction from pipeline 8 mixes.The product that comes out from high score 17 bottoms enters stabilizer tower 24 through pipeline 23, and gas is drawn through pipeline 25 from cat head, and liquid is drawn through pipeline 26 at the bottom of tower, mixes the back with petroleum naphtha fraction from pipeline 6 and goes out device as gasoline products through pipeline 27.
The following examples will give further instruction to method provided by the invention, but therefore not limit the present invention.
With FCC gasoline A is raw material, its character such as table 1.Earlier raw material is cut, cut point is 75 ℃, heavy petrol fraction, hydrogen contact with octane value recovering catalyst earlier and react, and obtain gasoline products after light fraction oil is in harmonious proportion behind reaction effluent and the mercaptan removal, and octane value recovering processing condition and product property are as shown in table 2.
With FCC gasoline A is that heavy petrol fraction, hydrogen contacted with octane value recovering catalyst, selective hydrodesulfurization agent and carries out octane value recovering, desulphurization reaction after raw material cut according to embodiment 1 described method.Obtain gasoline products after light fraction oil is in harmonious proportion behind generation oil and the mercaptan removal behind the upgrading, processing condition and product property are as shown in table 2.
With FCC gasoline A is that heavy petrol fraction, hydrogen contacted with the selective desulfurization agent and carries out desulphurization reaction after raw material cut according to embodiment 1 described method.Obtain gasoline products after light fraction oil is in harmonious proportion behind generation oil and the mercaptan removal after the desulfurization, processing condition and product property are as shown in table 3.
With FCC gasoline A is after raw material cuts according to embodiment 1 described method, and heavy petrol fraction, hydrogen contact with selective hydrodesulfurization agent, octane value recovering catalyst and carries out desulfurization, octane value recovering reaction.Obtain gasoline products after light fraction oil is in harmonious proportion behind generation oil and the mercaptan removal behind the upgrading, processing condition and product property are as shown in table 3.
Table 1 stock oil character
| Project | Raw material A |
| Density, g/cm 3 | 0.724 |
| Boiling range, ℃ | 34～195 |
| Fluorescent method is formed, v% | |
| Stable hydrocarbon | 44.5 |
| Alkene | 41.2 |
| Aromatic hydrocarbons | 14.3 |
| Sulphur, ppm | 462 |
| ?RON | 90.6 |
Table 2 embodiment 1～2 product oil nature
Table 3 embodiment 3～4 product oil natures
Claims (2)
1. the processing method of a catalytic gasoline hydrogenation desulfurating and reducing olefinic hydrocarbon is characterized in that: comprise the following steps:
(1) whole-distillate gasoline is cut into light, weigh two fractions, cut point is 60～80 ℃, the cutting principle thiophene is cut in the heavy fraction;
(2) light fraction removes wherein mercaptan through alkali cleaning refining desulfurization alcohol;
(3) heavy fraction contacts with octane value recovering catalyst earlier with hydrogen, carries out isomerization, aromizing and building-up reactions;
(4) reaction effluent contacts with catalyst for selectively hydrodesulfurizing without separation again, carries out hydrodesulfurization reaction, separates hydrogenated oil and obtains lighter hydrocarbons and gasoline fraction, and hydrogen-rich gas recycles;
(5) the heavy petrol fraction behind the hydro-upgrading with refining after the petroleum naphtha fraction mix and obtain gasoline products;
Wherein the described reaction conditions of step (3) is hydrogen dividing potential drop 1.5～3.0MPa, 360～430 ℃ of temperature of reaction, volume space velocity 1.2～3.0h-1, hydrogen to oil volume ratio 200～600, and catalyzer is the gasoline octane rating restorative;
The described reaction conditions of step (4) is hydrogen dividing potential drop 1.5～3.0MPa, 240～320 ℃ of temperature of reaction, volume space velocity 2.4～6.0h-1, hydrogen to oil volume ratio 200～600, and catalyzer is the gasoline selective hydrodesulfurizationmodification restorative;
The whole-distillate gasoline raw material is catalytically cracked gasoline, coker gasoline, pyrolysis gasoline, pressure gasoline or its mixture;
Described octane value recovering catalyst is to be carrier with in aluminum oxide or the molecular sieve one or more, one or both VIB of load or VIII family metal are active ingredient, auxiliary agent is one or both oxide compounds in IIB family or the group of the lanthanides, by catalyst weight per-cent: active ingredient is 5～25%, auxiliary agent is 1～10%, and carrier is 74～94%;
Described catalyst for selectively hydrodesulfurizing is to be carrier with the aluminum oxide, and Mo and Co are reactive metal, and one or more among Ce, Mg, K, P, the F are auxiliary agent, by catalyst weight per-cent: MoO
3Be 7.0～18.0%, CoO is 1.0～6.0%, auxiliary agent is 0.2～10.2%, all the other are the carrier amount;
2. the processing method of catalytic gasoline hydrogenation desulfurating and reducing olefinic hydrocarbon according to claim 1 is characterized in that: step (3) and step (4) are carried out in a reactor, or carry out in two reactors; When using a reactor, octane value recovering catalyst is seated in the reactor epimere, and catalyst for selectively hydrodesulfurizing is seated in the reactor hypomere.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103447057A (en) * | 2012-05-31 | 2013-12-18 | 武汉科林精细化工有限公司 | Preparation method of pre-vulcanized selective hydrodesulfurization catalyst for FCC gasoline |
| WO2018072342A1 (en) * | 2016-10-21 | 2018-04-26 | 中国石油化工股份有限公司 | Petrol treatment method |
| WO2021021449A1 (en) * | 2019-07-31 | 2021-02-04 | Saudi Arabian Oil Company | Process to remove olefins from light hydrocarbon stream by mercaptanization followed by merox removal of mercaptans from the separated stream |
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| CN1465666A (en) * | 2002-06-27 | 2004-01-07 | 中国石油化工股份有限公司 | Method of heavily desulfurating and reducing olefinic hydrocarbon for gasoline |
| CN1670135A (en) * | 2005-02-17 | 2005-09-21 | 中国石油化工集团公司 | Method for modifying low-grade gasoline |
| CN101307254A (en) * | 2007-05-18 | 2008-11-19 | 中国石油化工股份有限公司 | Process for producing cleaning gasoline from poor-quality gasoline |
| CN101368111A (en) * | 2007-08-16 | 2009-02-18 | 中国石油天然气集团公司 | Hydrogenation modification method for catalytically cracked gasoline |
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2010
- 2010-03-26 CN CN2010101347459A patent/CN102199448A/en active Pending
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1465666A (en) * | 2002-06-27 | 2004-01-07 | 中国石油化工股份有限公司 | Method of heavily desulfurating and reducing olefinic hydrocarbon for gasoline |
| CN1670135A (en) * | 2005-02-17 | 2005-09-21 | 中国石油化工集团公司 | Method for modifying low-grade gasoline |
| CN101307254A (en) * | 2007-05-18 | 2008-11-19 | 中国石油化工股份有限公司 | Process for producing cleaning gasoline from poor-quality gasoline |
| CN101368111A (en) * | 2007-08-16 | 2009-02-18 | 中国石油天然气集团公司 | Hydrogenation modification method for catalytically cracked gasoline |
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103447057A (en) * | 2012-05-31 | 2013-12-18 | 武汉科林精细化工有限公司 | Preparation method of pre-vulcanized selective hydrodesulfurization catalyst for FCC gasoline |
| WO2018072342A1 (en) * | 2016-10-21 | 2018-04-26 | 中国石油化工股份有限公司 | Petrol treatment method |
| CN110088247A (en) * | 2016-10-21 | 2019-08-02 | 中国石油化工股份有限公司 | A kind of vapour oil treatment process |
| US11041131B2 (en) | 2016-10-21 | 2021-06-22 | China Petroleum & Chemical Corporation | Process for treating gasoline |
| CN110088247B (en) * | 2016-10-21 | 2021-10-08 | 中国石油化工股份有限公司 | Gasoline treatment method |
| WO2021021449A1 (en) * | 2019-07-31 | 2021-02-04 | Saudi Arabian Oil Company | Process to remove olefins from light hydrocarbon stream by mercaptanization followed by merox removal of mercaptans from the separated stream |
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Application publication date: 20110928 |