CN101875856B - Wax oil hydrogenated treatment and catalytic cracking combined method - Google Patents
Wax oil hydrogenated treatment and catalytic cracking combined method Download PDFInfo
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- CN101875856B CN101875856B CN 200910207389 CN200910207389A CN101875856B CN 101875856 B CN101875856 B CN 101875856B CN 200910207389 CN200910207389 CN 200910207389 CN 200910207389 A CN200910207389 A CN 200910207389A CN 101875856 B CN101875856 B CN 101875856B
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Abstract
The invention discloses a wax oil hydrogenated treatment and catalytic cracking combined method, which comprises the following steps of: performing hydrogenated reaction on hydrogenated treatment raw materials in the presence of hydrogen and hydrogenated treatment catalyst, performing gas-liquid separation on the hydrogenated reaction effluent, circulating the gas phase for the hydrogenated reaction, directly feeding the liquid phase into a catalytic cracking device without fractionation, and mixing dry gas and liquefied gas separated from the catalytic cracking reaction effluent, catalytic cracking heavy fraction formed by catalytically cracking gasoline and the hydrogenated treatment raw materials to perform hydrogenated reaction. Compared with the prior art, the method can produce maximum gasoline, meanwhile saves equipment investment, makes full use of reaction heat energy and reduces the production energy consumption.
Description
Technical field
The present invention relates to a kind of wax oil lightening method, specifically with hydrotreatment and catalytic cracking organic assembling, mainly produce the processing method of gasoline products take wax oil as raw material.
Background technology
At present, oil product market particularly will be the trend that continues rising to the demand of gasoline to the demand of light, middle matter oil product both at home and abroad, and is then on a declining curve to the demand of heavy oil product.Simultaneously, oil property variation increasingly in the world, environmental regulation is increasingly strict.Therefore, how can realize that the oil Refining Technologies that heavy oil lighting, resulting product can satisfy again the petrol and diesel oil product specification of continuous harshness has become one of technology of domestic and international oil Refining Technologies developer's focus development with the rational cost of less expensive.
Catalytic cracking (being called for short FCC) technique is one of Main Means of heavy oil lighting in the petroleum refining industry, strong because of its adaptability to raw material, added value of product is high, good in economic efficiency, in world refining industry, be used widely, being most important heavy oil lighting secondary processing means, also is one of world today's refining of petroleum technique with fastest developing speed.
In order to solve the market contradiction increasing and more and more less to the heavy demand for fuel to the light-end products demand, the raw material range of the FCC technique of tradition take wax oil as raw material is increasing, as mixes refining part coker gas oil (CGO), deasphalted oil (DAO), light cycle oil (LCO) even long residuum (AR) and vacuum residuum (VR) etc.But, owing to be subjected to the restriction of himself reaction mechanism and operational condition, when adopting FCC technique directly to process the higher heavy feed stock of sulphur, nitrogen and metal impurities content, its light oil yield obviously descends, the obvious variation of product selectivity, catalyst attrition obviously increases, and petrol and diesel oil product and catalysis sulfureous in flue gas content obviously increase, and the advantage of catalytic cracking has been subject to great inhibition.
For the problems referred to above, wax oil hydrogenation processing-catalytic cracking combined technique is a kind of good method.The hydrotreating of FCC feedstock technology not only can be removed most of sulphur, nitrogen, metal impurities, also can improve the cracking performance of charging, reduces the FCC operating severity; Improve product and distribute, improve the purpose product selectivity; Reduce dry gas and coke yield, improve the economy of FCC apparatus; Reduce purpose product sulphur content; Reduce SO in the regenerated flue gas
xAnd NO
xContent; Make FCC have the ability of the chargings inferior such as processing sulfur-bearing heavy oil, therefore, wax oil hydrogenation is processed and the combination process of catalytic cracking got widely application.
Existing wax oil hydrogenation is processed and catalytic cracking combined technique, at first be that catalytically cracked material carries out hydrotreatment, hydrogenated oil is isolated diesel oil distillate, remaining tail oil cut is as the catalytic cracking charging, carry out catalytic cracking reaction, product is dry gas, liquefied gas, gasoline, diesel oil and coke, and recycle stock carries out the catalysis freshening or mix with hydrotreated feed carrying out hydrotreatment, and catalytic slurry gets rid of outward or the partially catalyzed freshening.Above-mentioned wax oil hydrogenation is processed with catalytic cracking combined technique and is existed yield of gasoline low, and heat energy loss is large, the unfavorable factors such as facility investment height.
CN1896192A discloses a kind of wax oil hydrogenation and has processed and catalytic cracking combination process, the method enters hydrotreater together with wax oil and heavy catalytic cycle oil, catalytic cracking diesel oil, carry out hydrogenation reaction in the presence of hydrogen and hydrogenation catalyst, reaction product isolated obtains gas, hydrotreated naphtha, hydrogenated diesel oil and hydrogenation tail oil; Wherein hydrogenation tail oil enters catalytic cracking unit, in the presence of catalytic cracking catalyst, carry out cracking reaction, obtain dry gas, liquefied gas, catalytically cracked gasoline, catalytic cracking diesel oil, heavy catalytic cycle oil and slurry oil after separating, wherein catalytic cracking diesel oil and heavy catalytic cycle oil are to hydrotreater.The method has improved the yield of light oil, has reduced coke yield, has reduced sulfur content in gasoline, reduces aromaticity content and the sulphur content of diesel oil and improves its cetane value.But the method needs two cover fractionating systems, has increased investment cost; Because the process heat exchange, heat-energy losses is more, and slurry oil does not take full advantage of, and simultaneously, hydrotreater and catalytic cracking unit have diesel product, and comparatively speaking, the total recovery of gasoline and gas products will reduce.In addition, catalytic cracking diesel oil mixes with wax oil and carries out hydrotreatment, because hydrotreatment is as main purpose take the wax oil hydrogenation desulfurization, and be unwell to the comprehensive upgrading requirement of diesel oil distillate, merge when processing catalytic cracking diesel oil and can not obtain present acceptable diesel product, when particularly processing inferior raw material, more can not obtain qualified diesel product.
CN1382776A discloses the method for a kind of residual hydrocracking and catalytically cracking heavy oil, the method is carried out hydrogenation reaction with residual oil at hydrotreater, the hydrogenated residue of gained enters catalytic cracking unit with optional vacuum gas oil and carries out cracking reaction, the heavy cycle oil of catalytic cracking returns hydrotreater, and the thing that steams that the distillation slurry oil obtains returns hydrotreater.The method is organically joined together two devices, residual oil, heavy cycle oil and slurry oil can be converted into light-end products.There is the weak point identical with CN1896192A in the method.
US6,565,739 disclose the combination process of a kind of two-stage catalytic cracking and hydrotreatment.The method is that the heavy cycle oil of first paragraph catalytic cracking is after hydrotreatment, enter the second segment catalytic cracking unit and carry out cracking, two-stage catalytic cracking adopts dissimilar catalyzer for different material, but the method need to be with the independent hydrotreatment of heavy cycle oil, it is a lot of to increase plant investment, and only solve the high problem of catalytic cracking unit coke, little to the quality product increase rate.
US6,123,830 disclose the combination process of a kind of two-stage catalytic cracking and two hydrotreatments.Stock oil at first passes through first catalytic cracking unit, obtains petroleum naphtha, diesel oil and heavy oil; First catalytic heavy enters second hydrotreater and carries out hydrogenation (its hydrogen dividing potential drop will be higher than first hydrogenation unit), obtains second hydrogenation tail oil, and the part tail oil carries out hydrogenation delivering to first hydrogenation unit; Second hydrogenation tail oil to the second catalytic cracking unit carried out cracking.This combination process is comparatively complicated, comprises two hydrotreaters and two catalytic cracking unit, and long flow path, complicated operation are invested too high.
US5,770,044 disclose the combination process of a kind of catalytic cracking and hydrotreatment.The method is: fresh feed separates obtaining gas, petroleum naphtha and heavier product (comprising diesel oil and heavy cycle oil) after catalytic cracking; Behind hydrotreater of heavier product introduction, separate obtaining petroleum naphtha, diesel oil and hydrogenation tail oil; Catalytic cracking unit is returned in hydrogenation tail oil recirculation.This combination process has better solved coke yield height, the poor problem of diesel quality, but fresh feed does not directly carry out catalytic cracking through hydrotreatment, and the sulphur content that obtains gasoline products is higher.
CN1119397C discloses a kind of hydrogenation and catalystic cracking combined process for residual oil, in the method, residual oil and clarified oil enter residual hydrogenation equipment together, react in the presence of hydrogen and hydrogenation catalyst, and heavy cycle oil circulates in catalytic cracking unit inside; The slurry oil of reaction gained obtains clarified oil through the separator separation, is back to hydrogenation unit.But slurry oil enters the residual hydrocracking device, and the easy green coke thing in the slurry oil will increase the carbon deposit of hydrogenation catalyst, has reduced hydrogenation activity and the operational cycle of hydrogenation catalyst, and heavy cycle oil is inner in catalytic cracking unit.Therefore, this method is limited to reducing coke yield, improving the quality of products.
In wax oil hydrogenation processing and the catalytic cracking combined technique, the energy consumption of fractionation plant accounts for larger ratio, and the energy consumption that how to reduce fractionation plant is the content that needs emphasis to consider.
Summary of the invention
For the deficiencies in the prior art, the invention provides a kind of wax oil hydrogenation and process and catalytic cracking combination method, can maximum produce gasoline products, technological process is simple simultaneously, whole Energy Intensity Reduction.
Wax oil hydrogenation of the present invention is processed and catalytic cracking combination method comprises: hydrotreated feed is carried out hydrogenation reaction in the presence of hydrogen and hydrotreating catalyst, the hydrogenation reaction effluent gas-liquid separation, gas phase is cycled to used in hydrogenation reaction, liquid phase directly enters catalytic cracking unit without fractionation, and the catalytic cracking reaction effluent is isolated catalytic cracking last running behind dry gas, liquefied gas and the catalytically cracked gasoline and mixed with hydrotreated feed and carry out hydrogenation reaction.
In the inventive method, hydrotreated feed comprises the one or any mixing oil in straight run decompressed wax oil, wax tailings, the deasphalted oil.Hydrogenation reaction effluent at first carries out gas-liquid separation, this gas-liquid separation is carried out under the condition identical with the reaction pressure grade, separate the gas phase that obtains and be mainly hydrogen, through being cycled to used in hydrogenation reaction after the selectable depriving hydrogen sulphide processing, hydrogenation process needs to replenish new hydrogen simultaneously with the consumption of postreaction process.The liquid phase that obtains after the hydrogenation reaction effluent gas-liquid separation enters light pressure separator, then directly enters catalytic cracking unit.
In the inventive method, the catalyzer that hydrogenation process uses and processing condition can require to determine by the conventional knowledge in this area according to feedstock property and quality product.Typical hydrogenation reaction processing condition are: hydrogen dividing potential drop 8.0MPa～16.0MPa, 300 ℃～450 ℃ of temperature of reaction, volume space velocity 0.1h during liquid
-1～3.0h
-1, the volume ratio of hydrogen and liquid phase material (hereinafter to be referred as hydrogen-oil ratio) 300～2000.
In the inventive method, the hydrogenation catalyst that hydrotreating catalyst can be a kind of desulfurization, denitrogenation, the aromatic saturation ability is strong, its active metal component is tungsten-nickel, molybdenum-nickel, molybdenum-cobalt or tungsten-molybdenum-array modes such as nickel, carrier is aluminum oxide, silicon-dioxide or amorphous silicon aluminium, wherein aluminum oxide is the most frequently used carrier, can contain simultaneously suitable auxiliary agent in the hydrotreating catalyst, such as P, B, Ti, Zr, F etc., can adopt commercial catalyst, also can be by the existing method preparation in this area.If have higher metal content or carbon residue higher or the coking precursor amounts is higher in the raw material; in order to protect hydrotreating catalyst and to prolong running period; can be before hydrotreating catalyst contacts raw material placement part guard catalyst and/or catalyst for demetalation, its ratio is 5%～30% (volume) of hydrotreating catalyst.The hydrogenator type is fixed bed, and hydrogenation unit comprises a reactor at least, and hydrotreater does not arrange fractionating system.
In the inventive method, catalytic cracking can be adopted this area routine techniques.Catalytic cracking unit can be that every covering device should comprise a reactor, a revivifier at least more than a cover or overlapped.Catalytic cracking unit arranges separation column, can every cover catalytic cracking unit set respectively, also can share.Catalytic cracking fractionating tower is dry gas, liquefied gas, catalytically cracked gasoline and catalytic cracking last running with the fractionation of catalytic cracking reaction effluent.Catalytic cracking last running is carried out hydrogenation reaction after filtering out first the micro-catalytic cracking catalyst powder that contains.
Catalytic cracking catalyst and processing condition adopt this area routine techniques.Typical catalytic cracking catalyst contains REY, REHY, ZSM-5 molecular sieve catalyzer or mixture.Processing condition are: 630 ℃～800 ℃ of weight ratio (hereinafter to be referred as agent-oil ratio) 3～10, the regeneration temperatures of 470 ℃～570 ℃ of temperature of reaction, 0.5～5.0 second reaction times, catalyzer and stock oil, the stock oil here refers to enter the stock oil of catalytic cracking unit.
The concrete technology condition of hydrotreatment and catalytic cracking can be obtained by simple experiment according to feedstock property and product quality indicator by the technician.
The invention has the advantages that:
1, in whole combination process, main products is catalytically cracked gasoline, liquefied gas and a small amount of dry gas, thus can guarantee that maximum ground produces gasoline.
2, the catalytic cracking reaction effluent is not isolated catalytically cracked oil, has solved slurry oil goes out catalyst solid powder because viscosity is very much not easily separated problem.Contain diesel oil distillate in the catalytic cracking heavy distillate, because the diluting effect of diesel oil distillate, catalyst solid powder wherein filters to become and is more prone to, and has also reduced the hydrogenation reaction difficulty of hydrotreatment parallel feeding simultaneously.When isolating catalytically cracked oil, although can part utilize by clarification, utilization ratio is lower, and the inventive method does not produce and effluxes part owing to do not isolate catalytically cracked oil, has improved the utilization ratio of raw material.
3, from whole combination process, need not establish fractionating system in the hydrotreater, hydrotreatment generates oil and directly enters catalyst cracker, need not establish feedstock pump in the middle of it, catalytic cracking last running is played diluting effect to fresh wax oil raw material, thereby the conveying of mixing raw material oil and filtration are more prone to.The fractionating system of catalytic cracking reaction effluent only fractionates out the light-end productss such as gasoline fraction, and the required theoretical separation tray number of separation column reduces greatly.More than several aspects facility investment is greatly reduced.
4, because hydrotreater is not established fractionating system, hydrogenated oil directly enters catalyst cracker, catalytic cracking generates oil after isolating gas products and catalytic gasoline, the residue mixing oil loops back hydrogenation unit after filtering, above-mentioned two processes greatly reduce the loss of heat, greatly reduce simultaneously the required energy of fractionation process, thereby reduced the energy consumption of whole technological process.
Description of drawings
Fig. 1 is that wax oil hydrogenation of the present invention is processed and the catalytic cracking combination method process flow diagram.
Embodiment
Below in conjunction with accompanying drawing method provided by the present invention is further detailed, but does not therefore limit the present invention.
Technical process is described in detail as follows:
Catalytic cracking last running 18 after wax oil raw material 1 and the filtration mixes, boost after and recycle hydrogen 2 be mixed into hydrotreating reactor 4, by contacting with the hydrotreating catalyst bed, remove the impurity such as metal in the stock oil, sulphur, nitrogen, the reactions such as aromatic saturation, olefin saturated and mild cracking occur in imurity-removal.Because hydrotreatment is strong exothermal reaction, need in the middle of reactor bed, to introduce cold hydrogen 3, control temperature of reaction and temperature rise.Hydrotreating reactor 4 outlet reaction effluents 5 enter high-pressure separator 6 and carry out gas-liquid separation, isolated gaseous stream carries out being recycled to the hydrotreating reactor entrance after the laggard recycle compressors 9 of processing such as depriving hydrogen sulphide boost, the new hydrogen that replenishes also can be introduced after recycle compressor 9, isolated liquid phase stream arrives light pressure separator 7 more further to be separated, isolated liquid phase stream is without heat exchange and fractionation, adjust the pressure of light pressure separator, make liquid phase stream in the situation of not using feedstock pump, enter the reactive system 10 of catalytic cracking unit by pipeline 8.
Enter the reactive system 10 of catalytic cracking unit from the hydrogenated oil of pipeline 8, react at catalytic cracking catalyst, reacted oil gas logistics 11 enters the catalytic cracking fractionating tower 14 of catalytic unit, isolate gas 12 and catalytically cracked gasoline 13, gas 12 and catalytically cracked gasoline 13 dischargers, the remaining catalytic cracking last running 15 of separation column enters separator 16, the catalyst fines that filters out, mechanical impurity and solid particulate 17, the catalytic cracking last running 18 after the filtration is recycled to hydrotreater.
The following examples will further specify method provided by the invention, but not thereby limiting the invention.Used stock oil is the mixing oil of straight run decompressed wax oil and wax tailings in embodiment and the Comparative Examples, and its mass ratio is 50: 50, and its character is listed in table 1.Mixed gatch raw material hydropyrolysis experiment carries out in reactor, the filling hydrotreating catalyst, and hydrotreating catalyst is the commodity hydrotreating catalyst FF-14 of Fushun Petrochemical Research Institute's development and production.It is identical with used catalytic cracking catalyst in the Comparative Examples to execute example, is the catalytic cracking catalyst LBO-16 of Lanzhou Petrochemical Company Development and Production.
Comparative Examples
This Comparative Examples adopts conventional wax oil hydrogenation processing-catalyst cracking method, i.e. the raw material of hydrotreatment is the mixing oil of straight run decompressed wax oil and wax tailings, and catalytically cracked material is the hydrogenation wax oil, and heavy catalytic cycle oil is processed at the catalytic cracking unit internal recycle.Table 2, table 3, table 4 are respectively processing condition, product distributes and main products character.
Embodiment
This embodiment adopts wax oil hydrogenation provided by the invention to process and catalytic cracking combination method, will comprise that the catalytic cracking last running of catalytic cracking diesel oil, catalysis heavy cycle oil and catalytic slurry is circulated to further processing in the hydrotreater.Table 2, table 3, table 5 are respectively processing condition, product distributes and main products character.
Comparing result shows that after catalytic cracking heavy distillate and the processing of fresh wax oil raw material mixed hydrogenation, the catalytically cracked gasoline yield increases by 22.96 percentage points, and coke yield descends to some extent, and the yield of dry gas and liquefied gas increases.The method can satisfy the enterprise that wishes increasing gasoline yield well.
Table 1 stock oil character
| Density (20 ℃), g/cm 3 | 0.9237 |
| S, quality % | 1.95 |
| N，μg/g | 2542 |
| Carbon residue, quality % | 0.46 |
| Boiling range (D-1160), |
|
| 10％/50％ | 374/452 |
| 95%/do | 546/559 |
Table 2 hydrotreatment and catalytic cracking process condition
| Title | Comparative Examples | Embodiment |
| The hydroprocessing technique condition | ||
| Raw material | Fresh feed | Fresh feed+catalytic cracking last running |
| The hydrogen dividing potential drop, MPa | 8.0 | 8.0 |
| Temperature of reaction, ℃ | 375 | 375 |
| Volume space velocity ●，h -1 | 1.0 | 1.0 |
| Hydrogen-oil ratio | 800 | 800 |
| The catalytic cracking process condition | ||
| Raw material | The hydrogenation wax oil | The mixing oil hydrogenated oil |
| Temperature of reaction, ℃ | 500 | 500 |
| Agent-oil ratio ● | 5.4 | 5.4 |
● calculate with the device inlet amount.
Table 3 product distributes
| Title | Comparative Examples | Embodiment |
| The hydrotreatment product distributes ●: quality % | ||
| Chemical hydrogen consumption | 0.88 | 1.18 |
| Gas | 2.59 | 2.48 |
| Petroleum naphtha | 0 | - |
| Diesel oil | 20.57 | - |
| Hydrogenation tail oil | 77.72 | - |
| The catalytic cracking product distributes ●: quality % | ||
| Dry gas | 2.05 | 2.17 |
| Liquefied gas | 17.68 | 25.58 |
| Gasoline | 55.58 | 66.97 |
| Diesel oil | 16.12 | - |
| Heavy cycle oil | 0 | - |
| Coke | 8.57 | 5.28 |
| Two covering devices add up to ●●, quality % | ||
| Chemical hydrogen consumption | 0.88 | 1.18 |
| Dry gas | 4.18 | 4.54 |
| Liquefied gas | 13.74 | 25.27 |
| Gasoline (comprising hydrotreated naphtha) | 43.20 | 66.16 |
| Diesel oil | 33.10 | - |
| Coke | 6.66 | 5.21 |
● take the device inlet amount as 100% calculating, ● ● take fresh feed as 100% calculating.
The conventional wax oil hydrogenation processing-catalytic cracking of table 4 main products character
●
● wherein hydrogenation wax oil, heavy catalytic cycle oil are intermediates
Table 5 main products character of the present invention
| Product | Catalytically cracked gasoline |
| Density (20 ℃), g/cm 3 | 0.7368 |
| S，μg/g | 32.0 |
| RON | 90.0 |
Claims (9)
1. a hydrotreatment and catalytic cracking combination method, hydrotreated feed is carried out hydrogenation reaction in the presence of hydrogen and hydrotreating catalyst, it is characterized in that: the hydrogenation reaction effluent gas-liquid separation, gas phase is cycled to used in hydrogenation reaction, liquid phase directly enters catalytic cracking unit without fractionation, and the catalytic cracking reaction effluent is isolated catalytic cracking last running behind dry gas, liquefied gas and the catalytically cracked gasoline and mixed with hydrotreated feed and carry out hydrogenation reaction; Hydrotreated feed comprises the one or any mixing oil in straight run decompressed wax oil, wax tailings, the deasphalted oil.
2. in accordance with the method for claim 1, it is characterized in that: hydrogenation reaction effluent at first carries out gas-liquid separation, this gas-liquid separation is carried out under the condition identical with the reaction pressure grade, separate the gas phase that obtains and be mainly hydrogen, be cycled to used in hydrogenation reaction after processing through selectable depriving hydrogen sulphide.
3. in accordance with the method for claim 1, it is characterized in that: the liquid phase that obtains after the hydrogenation reaction effluent gas-liquid separation enters light pressure separator, then directly enters catalytic cracking unit.
4. in accordance with the method for claim 1, it is characterized in that: the hydrogenation reaction processing condition are: hydrogen dividing potential drop 8.0MPa～16.0MPa, 300 ℃～450 ℃ of temperature of reaction, volume space velocity 0.1h during liquid
-1～3.0h
-1, the volume ratio of hydrogen and liquid phase material is 300～2000.
5. in accordance with the method for claim 1, it is characterized in that: the active metal component of hydrotreating catalyst is tungsten-nickel, molybdenum-nickel, molybdenum-cobalt or tungsten-molybdenum-nickel array mode, and carrier is aluminum oxide, silicon-dioxide or amorphous silicon aluminium.
6. in accordance with the method for claim 1, it is characterized in that: placement part guard catalyst and/or catalyst for demetalation before hydrotreating catalyst contact raw material, its ratio is 5%～30% of hydrotreating catalyst volume.
7. in accordance with the method for claim 1, it is characterized in that: catalytic cracking unit is that every covering device should comprise a reactor, a revivifier at least more than a cover or overlapped, and catalytic cracking unit arranges separation column, every cover catalytic cracking unit arranges respectively separation column, perhaps shares separation column.
8. it is characterized in that in accordance with the method for claim 1: catalytic cracking last running is carried out hydrogenation reaction after filtering out first the micro-catalytic cracking catalyst powder that contains.
9. in accordance with the method for claim 1, it is characterized in that: catalytic cracking catalyst contains the mixture of REY, REHY, ZSM-5 molecular sieve catalyzer or above-mentioned molecular sieve, and the catalytic cracking process condition is: 630 ℃～800 ℃ of weight ratio 3～10, the regeneration temperatures of 470 ℃～570 ℃ of temperature of reaction, 0.5～5.0 second reaction times, catalyzer and stock oil.
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| CN109988645A (en) * | 2017-12-29 | 2019-07-09 | 中国石油化工股份有限公司 | A kind of hydro-upgrading of inferior diesel and hydrofinishing group technology |
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| CN103773495B (en) * | 2012-10-24 | 2016-01-13 | 中国石油化工股份有限公司 | A kind of hydrotreatment-catalytic cracking combination process |
| CN103773486B (en) * | 2012-10-24 | 2016-03-02 | 中国石油化工股份有限公司 | A kind of combined method of voluminous high-value product |
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| CN109988645B (en) * | 2017-12-29 | 2021-06-04 | 中国石油化工股份有限公司 | Hydrogenation modification and hydrofining combined process for inferior diesel oil |
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