CN101434865B - Heavy distillate hydrogenation and catalytic cracking combined method - Google Patents
Heavy distillate hydrogenation and catalytic cracking combined method Download PDFInfo
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Abstract
The invention relates to a combination method of hydrogenation disposal and catalytic cracking used for heavy distillate oil. Under the hydrogenation disposal condition, heavy distillate raw material oil and circular hydrogen are mixed and pass by a first hydrogenation disposal reaction area, thus generating oil which is separated in high-pressure separation to obtain gas and liquid; the gas is desulfurized and mixed with the liquid and then the mixture passes by a second hydrogenation disposal reaction area, thus generating the oil which is separated in a high-pressure separator to obtain the gas which enters a compressor and subsequently enters the first hydrogenation disposal reaction area; and the obtained liquid is fractionated to obtain the low-sulfur light oil product and heavy oil product. The heavy oil product can be independently catalytically cracked or mixed with other heavy raw material oils and then catalytically cracked, thus gaining various light oil products and circular oil; and the circular oil can be circulated and returned to the catalytic cracking process and also can enter the hydrogenation disposal process. Compared with the prior art, the method effectively improves the hydrogenation disposal depth of the raw material oil, needs only one circular hydrogenation system for two hydrogenation disposal reaction areas, has low investment of equipment, low operation expense, and can directly produce clean gasoline and diesel.
Description
Technical field
The present invention relates to a kind of combined method, particularly a kind of hydrotreatment and catalytic cracking combined method.Make full use of the low-sulfur recycle hydrogen; Heavy distillate inferior is carried out hydrotreatment; Hydrogenation tail oil is through obtaining meeting clean gasoline, diesel oil distillate and the high added value gas etc. of environmental regulation requirement behind the catalytic cracking process; Catalytic cracking recycle oil can circulate at CCU, also can all or part of entering hydrotreating reactor.
Background technology
Oil property becomes heavy gradually, becomes bad in the our times scope; The increasingly stringent of the sustainable development of world economy and environmental regulation in addition; Need to produce a large amount of light clean fuels; These all require existing oil Refining Technologies is improved, and produce satisfactory product with minimum cost.
Heavy feed stock in China is produced in the working method of light-end products, and catalytic cracking (FCC) still accounts for critical role.Along with the requirement of crude quality variation and environmental regulation, the clean cargo of catalytic cracking technology direct production are second-rate, and especially the sulphur content of catalytic gasoline is than higher, and catalytic diesel oil sulphur content and aromaticity content are high, cetane value is low.In order to improve the quality of catalytic cracking product, need certain processing means, topmost approach generally has two kinds, i.e. and catalytic cracking generates the pre-treatment that oil subsidy fills unifining and catalytically cracked material.Because FCC raw material hydrogenation preconditioning technique can be avoided the problem of loss of octane number in the catalytic gasoline hydrogenation treating process, and has following advantage: the replacing speed that can reduce the FCC catalyzer; Reduce the FCC coke yield; Improving the FCC product distributes, improves the purpose product yield, reduces non-purpose product yield; Directly improve the FCC quality product, reduce the product sulphur content; Reduce the quantity discharged of FCC revivifier SOx, NOx etc., so FCC raw material hydrogenation pretreatment technology is widely used in the refinery in modern times.
The catalytically cracked material preconditioning technique is that the raw oil with catalytic cracking carries out hydrotreatment earlier; Remove impurity such as wherein most of sulphur, nitrogen, aromatic hydrocarbons has obtained fractional saturation, thereby has improved the raw oil quality of catalytic cracking; So just reduced the operating severity of catalytic cracking; And improved the catalytic cracking quality product, and can directly obtain the purpose product, perhaps reduced back purified difficulty.
Although catalytic cracking technology along with the development of technology, all improves in every respect and innovates, still there is increasing problem in use separately.Existing catalytically cracked material preconditioning technique mainly contains: US3983029 and US6793804 disclose hydroprocessing technique and catalyzer; CN1313379 discloses a kind of hydroprocessing process of poor-quality raw material for catalytic cracking, and CN1646665 discloses the hydrotreatment of hydrocarbon raw material.These patents use conventional hydrotreating catalyst under the common process condition, to carry out hydrotreatment, adopt the single pass flow process usually, owing to receive the influence that raw oil becomes heavy variation day by day, only under the critical operation condition, could reduce the sulphur content of resultant.These patents all are for catalytic cracking provides hydrogenating materials oil, and undeclared and catalytic cracking combination use.
In the said patent of US4426276 and US3193488; Catalytic cracking and hydrogen cracking associating; Its flow process is for carrying out catalytic cracking with the long residuum of crude oil, and the purpose product is a gasoline, and the LCO in the reaction product and HCO (gently, heavy cycle oil) mix with the normal pressure intermediate oil and carry out hydrogen cracking; Hydrocracking tail oil or circulation or get into catalytic cracking or the oil that acts as a fuel, catalytically cracked oil effluxes.Its main purpose is maximum production gasoline.It is relatively poor that the subject matter of this technology is that long residuum carries out the gasoline product quality that catalytic cracking obtains, and can't satisfy the environmental requirement of increasingly stringent, and simultaneously along with the intermediate oil demand obviously increases, this technical process then needs further to improve.In addition; Because refinery's treatment capacity increases; And the heavy crude amount increases, the also corresponding increase of output of therefore heavy, residual oil, and this makes the development of means of this important light materialization of heavy oil of catalytic cracking receive restriction significantly; Need to improve the quality product of CCU, reduce its operating severity with other method.
Summary of the invention
Deficiency to prior art; The present invention provides a kind of heavy distillate Deep Hydrotreating and catalytic cracking combination method; Can under than the demulcent operational condition, effectively improve the hydrotreatment degree of depth; Production low-sulfur catalytic cracking stock; And the catalysis recycle stock returns hydrotreater, has the operating severity that reduces the hydrogenation pretreatment unit, reduces the operating operation expense, reduces temperature of reaction, increases the apparatus processes ability and prolongs hydrogenation catalyst work-ing life, improves catalytically cracked material character and improve characteristics such as catalytic cracking quality product.
Hydroprocessing process of the present invention comprises following content:
A) with the heavy distillate be raw oil, under the hydrotreatment operational condition, raw oil and hydrogen-rich gas are through the first hydrotreatment reaction zone;
B) hydrotreatment that obtains of step a is flowed out thing and is got into Separate System of Water-jet, separates obtaining gas and liquid;
C) gas that obtains of step b carries out depriving hydrogen sulphide and handles;
D) liquid that obtains of gas phase behind the depriving hydrogen sulphide that obtains of step c and step b is through the second hydrotreatment reaction zone;
E) hydrotreatment that obtains of steps d is flowed out thing and is got into separation system, separates obtaining gas, light ends and heavy ends;
F) gas that obtains of step e gets into the first hydrotreatment reaction zone behind circulating hydrogen compressor, and as the hydrogen source of the first hydrotreatment reaction zone, the liquid product that step e obtains comprises low-sulfur petroleum naphtha and low-sulfur diesel-oil, and the low-sulfur wax oil;
G) the low-sulfur wax oil with step f carries out catalytic cracking, directly obtains gas, gasoline, diesel oil, recycle stock and slurry oil.
It is 350～600 ℃ of heavy endss that the heavy distillate raw material that the inventive method is used generally comprises boiling range; Adding can be in the various vacuum gas oils (VGO) that obtain in the petroleum refining process, deasphalted oil (DAO) coker gas oil (CGO), heavy cycle oil (HCO) etc. one or more, also can be from coal tar, gelatin liquefaction wet goods; Also can comprise residual oil (normal slag or subtract slag), flow process is unrestricted.These heavy distillates can all get into hydrotreater, also can select part to get into CCU (if residual oil is arranged then get into CCU).
The operational condition of the first hydrotreatment reaction zone is generally reaction pressure 3.0～20.0MPa, and hydrogen to oil volume ratio is 200: 1～2500: 1, and volume space velocity is 0.1～8.0h
-1, 260 ℃～455 ℃ of temperature of reaction; Preferred operational condition is reaction pressure 4.0～18.0MPa, hydrogen to oil volume ratio 300: 1～2000: 1, volume space velocity 0.2～6.0h
-1, 280～444 ℃ of temperature of reaction.The operational condition of the second hydrotreatment reaction zone is generally reaction pressure 3.0～20.0MPa, and hydrogen to oil volume ratio is 200: 1～2500: 1, and volume space velocity is 0.1～8.0h
-1, 260 ℃～455 ℃ of temperature of reaction; Preferred operational condition is reaction pressure 4.0～18.0MPa, hydrogen to oil volume ratio 300: 1～2000: 1, volume space velocity 0.2～6.0h
-1, 280～444 ℃ of temperature of reaction.First reaction zone is low than second reaction zone pressure, general high 0.01～2.0MPa.
Two hydrotreatment reaction zones of the present invention can use identical hydrotreating catalyst, also can use different hydrotreating catalysts.Hydrotreating catalyst can all be conventional hydrotreating catalyst, also can be the combination of conventional hydrotreating catalyst and bulk phase catalyst.During combination loading; Bulk phase catalyst can be seated in the top of reaction zone, also can be seated in the bottom of reaction zone, and perhaps two types catalyzer loads at interval; The volume ratio of bulk phase catalyst and conventional catalyst is 90: 10～10: 90, preferred 20: 80～80: 20.During combination loading, preferred feed through the bulk phase catalyst bed, helps bringing into play the catalyzer overall activity most then at first through common hydrotreating catalyst bed.Wherein conventional hydrotreating catalyst can be various commercial catalysts; As Fushun Petrochemical Research Institute (FRIPP) development and production 3926,3936, hydrotreating catalyst such as CH-20,3996, FF-14, FF-16, FF-18, FF-26; Catalyzer such as the HR-416 of Inst Francais Du Petrole, HR-448; The TK-525 of Topsor company, TK-557 catalyzer, the KF-752 of AKZO company, KF-840, KF-901, KF-907 or the like.The FH-FS of bulk phase catalyst such as Fushun Petrochemical Research Institute (FRIPP) development and production etc.Above-mentioned hydrotreating catalyst also can prepare by this area knowledge; Common hydrotreating catalyst (loaded catalyst; Active metallic content is relatively low, generally counts 20%～45% with oxide compound) the general support of the catalyst of preparation earlier, use pickling process supported active metal component then; Bulk phase catalyst (active metallic content is high, generally counts 50%～85% with oxide compound) generally adopts the coprecipitation method preparation.
A most important course of processing in the catalytic cracking technology crude oil secondary processing, but quality product is not high, does not meet the requirement of the environmental regulation of increasingly stringent.For improving the catalytic cracking quality product, technology of the present invention is taked to realize with the method for hydrotreater material cooperation, adjustment charging.Technology catalytically cracked material hydrogenation tail oil of the present invention also can be mixed and refine not other heavy feed stock of hydrogenation.CCU comprises catalyst cracker and catalytic fractionator two portions.The operational condition of catalyst cracker is: 450 ℃～550 ℃ of average reaction temperature, best 480 ℃～520 ℃; Agent weight of oil ratio is 2～30, best 3～20; With catalyzer duration of contact be 0.5 second～15 seconds, best 0.5 second～5 seconds; Reaction pressure is 0.1～0.5MPa, best 0.1～0.3MPa.Catalytic fractionator can be produced low-density oil cut product and catalytic cracking tail oils such as liquefied gas, light naphthar, heavy naphtha, aviation kerosene, diesel oil, and wherein the yield of catalytic cracking tail oil is 5wt%～80wt%, and preferably yield is 10wt%～50wt%.The catalytic cracking tail oil comprises recycle stock and slurry oil, and all or part of entering hydrotreatment reaction zone of recycle stock can get into the first hydrotreatment reaction zone, also can get into the second hydrotreatment reaction zone, preferably gets into the first hydrotreatment reaction zone.Slurry oil removes that catalyst powder is last also can the above-mentioned hydrotreatment reaction zone of all or part of entering.The concrete operations condition can be confirmed by the logical real simple experiment of this area general knowledge according to feedstock property and quality product requirement.
Compared with prior art; Characteristics of the present invention are: because the present invention has increased a hydrotreating reactor; First section hydrotreatment generates oil under hydrogen and low in hydrogen sulphide atmosphere; Can reach the effect of deep desulfuration, perhaps reach identical when desulphurizing activated, improve the treatment capacity of hydrotreater.Because a circulating hydrogen compressor and a cover product fractionating system are only used in hydrotreatment, the circulating hydrogen compressor load reduces by 50% when reaching identical hydrogen-oil ratio, therefore can significantly reduce facility investment and process cost.Particularly with the CCU organic assembling after, can substantially improve CCU charging quality, thereby effectively improve quality producies such as catalytically cracked gasoline, diesel oil.
Description of drawings
Fig. 1 is a kind of process flow diagram of the present invention.
Fig. 2 is an another kind of process flow diagram of the present invention.
Embodiment
Shown in Figure 1; At first poor heavy raw material oil 1 and second reaction zone obtains hydrogen-rich gas 3 and is mixed into first reaction zone 2, and the first hydrotreatment logistics 4 that obtains separates in separator 5, separates the gas 6 and liquid 7 that obtain; Wherein gas 6 after thionizer 8 desulfurization as the hydrogen 10 of second reaction zone; Liquid 7 is mixed into second reaction zone 11 with hydrogen 10, obtains the second hydrotreatment logistics 12 after the reaction and in separator 13, separates, and separates obtaining gas, light ends 14 and hydrogenation wax oil 15.Light ends 14 can be used as clean cargo; Hydrogenation wax oil 15 is as the CCU charging; Gas mixes the hydrogen source as first reaction zone with new hydrogen 16 after circulating hydrogen compressor 9 superchargings; Hydrogenation wax oil 15 gets into catalyst cracker 17 with other heavy raw oil 26; The catalytic cracking that obtains generates oil fractionation in separation column 19 and obtains gas 20, gasoline 21 and diesel oil 22 (light cycle oil), slurry oil 23 and turning oil, and wherein turning oil can all or part of circulation get into hydrotreatment first reactor drum 2 as 24, also can partly loop back catalyst cracker 17.
Fig. 2 is merely with Fig. 1 difference: new hydrogen 16 mixes directly entering second reaction zone 11 with processed gas 10.
Through embodiment the present invention program and effect are described below.
Table 1 raw oil character
| The raw oil title | Raw oil-1 * | Raw oil-2 ** |
| Density (20 ℃)/gcm -3 | 0.931 | 0.902 |
| The boiling range scope/℃ | 360～600 | 360～560 |
| Sulphur content, wt% | 3.10 | 1.60 |
| Aromaticity content, wt% | 58 | 43 |
*Raw oil-1 is mixing oil (VGO: CGO: DAO=50 wherein: 25: 25 weight ratios)
*Raw oil-2 is mixing oil (VGO: CGO=60 wherein: 40 weight ratios)
The catalyzer that hydrotreatment is used is 3936 and FF-14, produces by Fushun Petrochemical Research Institute.
The main composition and the character of table 2 hydrotreating catalyst
| Catalyzer | 3936 | FF-14 |
| Catalyzer is formed | ||
| MoO 3，wt％ | 24.5 | 24.0 |
| NiO，wt％ | 3.8 | 2.0 |
| CoO，wt％ | - | 1.6 |
| Carrier, wt% | Surplus | Surplus |
| The main character of catalyzer | ||
| Specific surface/m 2·g -1 | ＞160 | ＞160 |
| Pore volume/mlg -1 | 0.33 | ＞0.30 |
Table 3 embodiment hydroprocessing technique condition and test-results
| | Embodiment | 1 | |
|
|
| First reactor drum | ||||
| Catalyzer | FF-14 | FF-14 | 3936 | 3936 |
| Raw oil | Raw oil-1 | Raw oil-2 and catalytic cracking recycle oil | Raw oil-1 and catalytic cracking recycle oil | Raw oil-2 |
| The raw oil ratio | - | 80∶20 | 85∶15 | - |
| Pressure/MPa | 8.0 | 14.0 | 10.0 | 6.0 |
| The inlet hydrogen to oil volume ratio | 600∶1 | 600∶1 | 1000∶1 | 400∶1 |
| Air speed/h -1 | 2.0 | 3.0 | 1.5 | 1.0 |
| Temperature/℃ | 370 | 385 | 355 | 350 |
| Second reactor drum | ||||
| Catalyzer | FF-14 | FF-14 | 3936 | 3936 |
| Raw oil | The one anti-oil that generates | The one anti-oil that generates | The one anti-oil that generates | The one anti-oil that generates |
| Pressure/MPa | 9.0 | 15.0 | 10.5 | 7.0 |
| The inlet hydrogen to oil volume ratio | 600∶1 | 600∶1 | 1000∶1 | 400∶1 |
| Air speed/h -1 | 2.0 | 5.0 | 5.0 | 3.0 |
| Temperature/℃ | 360 | 370 | 340 | 360 |
| Hydrogenation wax oil sulphur content/μ gg -1 | 1000 | 160 | 950 | 470 |
Hydrotreatment generates oil entering CCU and processes.Catalytic cracking catalyst is the CC-16 catalytic cracking catalyst that Chang Ling oil-refining chemical head factory is produced.
Table 4 embodiment catalytic cracking process condition and product property
| |
|
|
|
|
| Fresh feed oil | The hydrogenation wax oil | The hydrogenation wax oil | The hydrogenation wax oil | Hydrogenation wax oil and |
| The raw oil ratio | - | - | - | 90∶10 |
| Temperature of reaction/℃ | 510 | 500 | 500 | 490 |
| Pressure/MPa | 0.25 | 0.25 | 0.25 | 0.25 |
| Agent- |
5 | 5 | 6 | 6 |
| Finish duration of contact/ |
3 | 3 | 3 | 3 |
| Product distributes and product property | ||||
| Dry gas, wt% | 1.4 | 1.4 | 1.8 | 1.5 |
| Liquefied gas, wt% | 22.4 | 16.7 | 17.8 | 24.5 |
| Gasoline, wt% | 58.5 | 50.8 | 49.5 | 56.5 |
| Diesel oil, wt% | 13.8 | 12.9 | 13.4 | 14.8 |
| Advance the recycle stock of hydrogenation, wt% | - | 13.0 | 11.2 | - |
| Coke, wt% | 1.3 | 1.2 | 2.4 | 2.2 |
| Content of sulfur in gasoline/μ gg -1 | 45 | 5 | 35 | 220 |
| Diesel oil sulphur content/μ gg -1 | 1100 | 21?0 | 980 | 2000 |
Can find out through top embodiment; Owing to make full use of low in hydrogen sulphide atmosphere in hydrotreater second reaction zone; Reach the effect of deep desulfuration, behind catalytic cracking combined technique, can effectively improve the yield and the quality of improving clean cargo of light-end products.
Claims (13)
1. heavy distillate hydrotreatment and catalytic cracking combination method comprise following content:
A) with the heavy distillate be raw oil, under the hydrotreatment operational condition, raw oil and hydrogen-rich gas are through the first hydrotreatment reaction zone;
B) hydrotreatment that obtains of step a is flowed out thing and is got into Separate System of Water-jet, separates obtaining gas and liquid;
C) gas that obtains of step b carries out depriving hydrogen sulphide and handles;
D) liquid that obtains of gas phase behind the depriving hydrogen sulphide that obtains of step c and step b is through the second hydrotreatment reaction zone;
E) hydrotreatment that obtains of steps d is flowed out thing and is got into separation system, separates obtaining gas, light ends and heavy ends;
F) gas that obtains of step e gets into the first hydrotreatment reaction zone behind circulating hydrogen compressor, and as the hydrogen source of the first hydrotreatment reaction zone, the liquid product that step e obtains comprises low-sulfur petroleum naphtha and low-sulfur diesel-oil, and the low-sulfur wax oil;
G) the low-sulfur wax oil with step f carries out catalytic cracking, directly obtains gas, gasoline, diesel oil, recycle stock and slurry oil.
2. according to the described method of claim 1, it is characterized in that described heavy distillate raw material comprises that boiling range is 350～620 ℃ of heavy endss.
3. according to claim 1 or 2 described methods, it is characterized in that described heavy distillate raw material is one or more in vacuum gas oil, deasphalted oil, coker gas oil, the heavy cycle oil, perhaps from coal tar or liquefied coal coil.
4. according to the described method of claim 1, the operational condition that it is characterized in that the described first hydrotreatment reaction zone is reaction pressure 3.0～20.0MPa, and hydrogen to oil volume ratio is 200: 1～2500: 1, and volume space velocity is 0.1～8.0h
-1, 260 ℃～455 ℃ of temperature of reaction.
5. according to the described method of claim 1, the operational condition that it is characterized in that the described first hydrotreatment reaction zone is reaction pressure 4.0～18.0MPa, hydrogen to oil volume ratio 300: 1～2000: 1, volume space velocity 0.2～6.0h
-1, 280～444 ℃ of temperature of reaction.
6. according to the described method of claim 1, the operational condition that it is characterized in that the described second hydrotreatment reaction zone is reaction pressure 3.0～20.0MPa, and hydrogen to oil volume ratio is 200: 1～2500: 1, and volume space velocity is 0.1～8.0h
-1, 260 ℃～455 ℃ of temperature of reaction.
7. according to the described method of claim 1, the operational condition that it is characterized in that the described second hydrotreatment reaction zone is reaction pressure 4.0～18.0MPa, hydrogen to oil volume ratio 300: 1～2000: 1, volume space velocity 0.2～6.0h
-1, 280～444 ℃ of temperature of reaction.
8. according to the described method of claim 1, it is characterized in that the described first hydrotreatment reaction zone is lower than the second hydrotreatment reaction zone pressure, pressure difference value is 0.01～2.0MPa.
9. according to the described method of claim 1, it is characterized in that the described first hydrotreatment reaction zone uses identical hydrotreating catalyst with the second hydrotreatment reaction zone, perhaps uses different hydrotreating catalysts.
10. according to the described method of claim 9, it is characterized in that described hydrotreating catalyst is conventional hydrotreating catalyst, perhaps is the combination of conventional hydrotreating catalyst and bulk phase catalyst.
11. according to the described method of claim 1, it is characterized in that described Hydrocarbon Content by Catalytic Cracking Operation condition is 450 ℃～550 ℃ of temperature of reaction, agent weight of oil ratio is 2～30, with catalyzer duration of contact be 0.5 second～15 seconds, reaction pressure is 0.1～0.5MPa.
12. according to the described method of claim 1, it is characterized in that all or part of entering first hydrotreatment reaction zone of described catalytic cracking recycle oil, perhaps get into the second hydrotreatment reaction zone.
13., it is characterized in that described catalytically cracked oil removes the last all or part of entering first hydrotreatment reaction zone of catalyst powder, perhaps gets into the second hydrotreatment reaction zone according to the described method of claim 1.
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| CN109988625B (en) * | 2017-12-29 | 2021-06-04 | 中国石油化工股份有限公司 | Hydrofining and hydrocracking combined process |
Citations (4)
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|---|---|---|---|---|
| US3155608A (en) * | 1960-12-01 | 1964-11-03 | Exxon Research Engineering Co | Process for reducing metals content of catalytic cracking feedstock |
| CN1432629A (en) * | 2001-12-17 | 2003-07-30 | 切夫里昂美国公司 | Production process of high-quality middle cut |
| CN1982418A (en) * | 2005-12-14 | 2007-06-20 | 中国石油化工股份有限公司 | Production of cleaning fuel from heavy-fraction oil |
| CN101063047A (en) * | 2006-04-28 | 2007-10-31 | 中国石油化工股份有限公司 | Method of dense raw material hydrotreatment-catalytic cracking for improving propylene productivity |
-
2007
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Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3155608A (en) * | 1960-12-01 | 1964-11-03 | Exxon Research Engineering Co | Process for reducing metals content of catalytic cracking feedstock |
| CN1432629A (en) * | 2001-12-17 | 2003-07-30 | 切夫里昂美国公司 | Production process of high-quality middle cut |
| CN1982418A (en) * | 2005-12-14 | 2007-06-20 | 中国石油化工股份有限公司 | Production of cleaning fuel from heavy-fraction oil |
| CN101063047A (en) * | 2006-04-28 | 2007-10-31 | 中国石油化工股份有限公司 | Method of dense raw material hydrotreatment-catalytic cracking for improving propylene productivity |
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