CN1075549C - Method for producing base oil of high viscosity index lubricant - Google Patents
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- CN1075549C CN1075549C CN99113304A CN99113304A CN1075549C CN 1075549 C CN1075549 C CN 1075549C CN 99113304 A CN99113304 A CN 99113304A CN 99113304 A CN99113304 A CN 99113304A CN 1075549 C CN1075549 C CN 1075549C
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Abstract
The present invention relates to a method for producing base oil of a low pour point and high viscosity index lubricant, namely that hydrocarbon oil containing wax is taken as a raw material, and the purposes of the reduction of base oil pour points and the maintenance of high viscosity indexes can be achieved by the hydroisomerization of the wax. A hydroisomerizing reactor contains two sections of catalysts which are in series connection, and the catalysts respectively contain two different molecular sieve components and platinum or palladium hydrogenation dehydrogenation components.
Description
The present invention relates to the production method of a kind of low pour point, base oil of high viscosity index lubricant.
About produce the existing a large amount of patent and the bibliographical informations of method of low pour point, base oil of high viscosity index lubricant with the hydrocarbon raw material of the content of wax, its basic guiding theory all is that the acidity of shape selectivity by molecular sieve component in the heterogeneous catalyst and appropriateness is equipped with the stronger hydrogenation-dehydrogenation of noble metal component and heterogeneous activity the wax molecule (mainly being normal paraffin) of high pour point, high viscosity index (HVI) is carried out hydroisomerizing, and the isoparaffin that generates with one or two methyl chains reaches the purpose that reduces pour point and keep higher viscosity index.For example, nC
20Fusing point be that 36.6 ℃, viscosity index are 174, and iC
20Fusing point be 164 for-2.5 ℃, viscosity index, and the position of the isoparaffin side chain that obtains is low more the closer to main chain central authorities pour point.Therefore patent has in the past been mentioned and has been adopted the mordenite with shape selectivity, SAPO-11, SAPO-31, SAPO-41, ZSM-22, ZSM-23, mesoporous molecular sieves such as SSZ-32 are as the acidic components of heterogeneous catalyst, but, when adopting separately intermediate pore molecular sieve catalyst that the hydrocarbon feed of the content of wax is carried out isomerization dewaxing, because the pore volume of catalyzer, surface-area is less, make isomerization reaction be subjected to diffusion control, particularly higher or cut is heavier when the wax content of raw material, when aromaticity content is higher, then need harsh reaction conditions if will reach lower pour point, so not only can reduce base oil yield, also can accelerate the inactivation of catalyzer because of the over-drastic hydrocracking reaction takes place.
U.S.5,149,421 mention Pt/SAPO-11 connected to make in same reactor with the Pt/ZSM-5 catalyzer and are used for reaching lower pour point, but because the Pt/ZSM-5 catalyzer can be cracked into the wax molecule micro-molecular gas hydro carbons of low value, therefore, this method can cause the loss of base oil yield and viscosity index.
U.S.4,419,220 and 4,518,485 mention the isomerization dewaxing that carries out content of wax hydrocarbon ils with high silicon beta-molecular sieve, when transformation efficiency is low, the beta-molecular sieve catalyzer shows isomery selectivity preferably to normal paraffin, but, along with the raising of transformation efficiency, owing to do not have space constraint in the large pore molecular sieve duct, easily generate highly-branched chain isomerous body, these highly-branched chain isomerous bodies are little to reducing the pour point contribution, and cracking easily, cause the loss of base oil yield.Therefore, must be controlled under the lower transformation efficiency and just can obtain higher base oil yield, in order to reach lower pour point, also need adopt the method for solvent dewaxing or catalytic dewaxing further to reduce wax content in the base oil, thereby cause the decline of base oil yield and viscosity index.
It is that the effluent after first section hydrotreatment is removed light oil distillate through separation that the two-stage hydrogenation method that CN1140199 mentions is produced lubricant base technology, heavy oil fraction is sent into second section reactor carry out isomerization dewaxing.
U.S.5,110,445 have introduced a kind of two-stage process process of producing high viscosity index (HVI), low pour point lubricant base, and the first step is that the catalyzer of content of wax hydrocarbon oil feed through containing beta-molecular sieve carries out hydroisomerizing, and second step was that solvent dewaxing further reduces pour point.
U.S.4,919,788 and EP0,225,053 have also introduced a kind of two-stage process process of producing low pour point, base oil of high viscosity index lubricant.The isomerization dewaxing catalyst that first section use contains platinum and high silicon beta-molecular sieve drops to the pour point of content of wax hydrocarbon feed higher about 11 ℃ than target pour point, and second section is adopted Ni/ZSM-5 or catalytic dewaxing catalysts such as ZSM-22, ZSM-23 carry out the selectivity catalytic dewaxing or solvent dewaxing further reduces pour point.
U.S.4,601,993 introduce a kind of precious metal dewaxing catalyst that contains two kinds of different pore size molecular sieve mixtures, the noble metal catalyst that is mixed and made into as the ZSM-5 of low tart beta-molecular sieve of macropore and mesopore, this macropore is mixed shape selectivity that the method for using is unfavorable for bringing into play mesoporous molecular sieve and the large pore molecular sieve isomery performance when the low-conversion with mesoporous molecular sieve, therefore can cause the loss of base oil yield and viscosity index.
U.S.4,599,162 have introduced a kind of dual catalyst serial hydrogenation dewaxing technique, and it is 2～12 mesoporous molecular sieve that first section catalyzer contains restricted index, and the restricted index of second section employed mesoporous molecular sieve of catalyzer is not less than 2.For example, first section is used Pt/ZSM-12/ZSM-23 to carry out isomerization dewaxing, and second section is used the Ni/ZSM-5 catalyzer to carry out catalytic dewaxing.Because the effect of Ni/ZSM-5 catalyzer is that the wax molecule that first section heterogeneous catalyst do not have to transform is cracked into the purpose that the micro-molecular gas hydrocarbon reaches further reduction pour point, certainly will cause the loss of base oil yield and viscosity index.
CN1137059 introduces a kind of hydrocracking tail oil two-stage dewaxing and produces lubricant base technology, first section hydrotreating catalyst mentioned and can be used beta-molecular sieve, second section is the isomerization catalyst that contains mesoporous molecular sieves such as SAPO-11, because first section catalyzer will be operated, therefore must use two reactors under lower temperature.And this patent is thought first section preferred Y zeolite catalyzer.Do not do for the character of beta-molecular sieve and to specify.
Though two step hydrogenating conversion process of above-mentioned prior art improve to some extent for aspects such as improving base oil yield, reduction pour point and maintenance viscosity higher index, still allow some leeway for the efficient of improving one's methods.Specifically, can make it help the isomerization reaction of wax molecule more to the acidity adjustment of first section employed macropore beta-molecular sieve of isomerization dewaxing catalyst, and lytic activity is very low, and first section transformation efficiency is controlled at lower level, so just first section catalyzer can be connected with the second section catalyzer that contains the SAPO-11 mesoporous molecular sieve and be contained in the same reactor, feasible operation is easier, and economy is stronger.
The object of the invention is to provide a kind of processing method of easy and simple to handle, preparation lubricant base that economy is strong.
The present invention program is: the two-stage catalytic agent is loaded in series connection in a reactor, in the presence of hydrogen, content of wax hydrocarbon oil crude material is contacted with beds, and effluent can obtain the lubricant base of fine intermediate oil and low pour point, high viscosity index (HVI) through fractionation.
First section is used the low tart beta-molecular sieve catalyzer of high silicon, and the lower transformation efficiency of control, the isomerization dewaxing catalyst that second section use contains mesopore SAPO-11 molecular sieve reaches the target pour point, what take place is the isomerization reaction of wax molecule because first section beta-molecular sieve catalyzer is main under lower transformation efficiency, and can remove impurity such as S, N in the raw material and aromatic hydrocarbons, thereby reduced the load of SAPO-11 catalyzer, made second section catalyzer be issued to the purpose pour point in lower temperature of reaction.Because mesopore SAPO-11 molecular sieve has shape selectivity preferably to the wax molecule, the isomery molecule that generates in first section is difficult for taking place the second pyrolysis reaction, therefore can guarantee higher viscosity index and base oil yield.
Beta-molecular sieve catalyzer after the modification has lower lytic activity, can connect with the SAPO-11 molecular sieve catalyst to be seated in the reactor, simplifies technical process, and economy is stronger.
So, the present invention relates to the production method of a kind of low pour point, high viscosity index (HVI) base oil, promptly content of wax hydrocarbon oil crude material contacts with hydrogen in the reactor that two sections placed in-line beds are housed.Wherein first section catalyzer contains high silicon, low tart macropore beta-molecular sieve and at least a VIII family noble metal component.The silica alumina ratio of first section employed beta-molecular sieve of catalyzer and acidity can and exchange the method that goes up basic metal or alkaline-earth metal ions by traditional hydrothermal treatment consists, acid treatment and control.Its silica alumina ratio greater than 70: 1, better be greater than 100: 1, more preferably greater than 200: 1.Second section catalyzer contains SAPO-11 molecular sieve and at least a VIII family noble metal component.The molar fraction (Si/Si+Al+P) of the second section employed SAPO-11 molecular sieve of catalyzer silicon is 0.03～0.30, is preferably 0.17～0.25, and crystal grain＜0.5 μ, is preferably 0.05～0.10 μ.And, two kinds of activity of such catalysts are mated preferably by adjusting the filling ratio of first section catalyzer and second section catalyzer.
First section and the second section employed VIII of catalyzer family precious metal are platinum and/or palladium component.The content of noble metal component in catalyzer is 0.1～10wt%, is preferably 0.2～5wt% (in element).
First section and second section catalyzer are except employed molecular sieve component, also comprise resistant to elevated temperatures oxide carrier, can be any inorganic oxide or its combination, selectively mix with the inert binder material arbitrarily, the example of suitable refractory oxide comprises two or more mixtures of aluminum oxide, silicon-dioxide, titanium oxide, zirconium white, boron oxide, silica-alumina, fluorided alumina, fluorinated silica-aluminum oxide and these materials.
The per-cent that first section catalyzer accounts for whole catalyst volumes is 3～20%, is preferably 5～15%.The per-cent that second section catalyzer accounts for whole catalyst volumes is 80～97%, is preferably 85～95%.Inventing employed proper raw material is the waxy hydrocarbon oil plant that boiling point to small part is higher than lubricant base, particularly suitable raw material has VGO hydrocracking tail oil, solvent-refined oil hydrotreatment tail oil, boiling range is generally 250～620 ℃, preferably 310～550 ℃.Also can use hydrotreatment tail oil and the slack wax and the soft wax etc. of propane deasphalting oil.
The operational condition of isomerization dewaxing is relevant with the purpose pour point that used feedstock property and requirement reach.In general, service temperature is 250～500 ℃, and preferred 320～400 ℃, working pressure is 1.0～25.0MPa, preferred 4.0～16.0MPa, and total liquid hourly space velocity (LHSV) is 0.1～10h
-1, preferred 0.5～5h
-1, hydrogen to oil volume ratio is 100～2000, is preferably 500～1500.
In general, adopt the final lubricant base that obtains of method of the present invention to have at least 100, preferred 110, more preferably at least 120 viscosity index and-9 ℃ or following, preferred-15 ℃ or following pour point.
First section of the inventive method used macropore, high silicon, low tart beta-molecular sieve catalyzer, and the lower transformation efficiency of control, and the isomerization dewaxing catalyst that second section use contains mesoporous molecular sieve such as SAPO-11 reaches the target pour point.The acidity of first section beta-molecular sieve catalyzer of control can suitably improve its temperature of reaction and is unlikely excessive fragmentation.In addition because the hydrogenating function of first section catalyst metal components, can remove impurity such as sulphur in the raw material, nitrogen largely, and making condensed-nuclei aromatics saturated, purpose is to reduce the load of SAPO-11 catalyzer, makes second section catalyzer can be issued to the purpose pour point in lower temperature of reaction.Acidity to first section employed macropore beta-molecular sieve of isomerization dewaxing catalyst is adjusted, reduce its lytic activity, it is operated under comparatively high temps, so just first section catalyzer can be connected with the second section catalyzer that contains mesoporous molecular sieves such as SAPO-11 and be contained in the same reactor, feasible operation is easier, and economy is stronger.Use this method, can produce the lube base of high viscosity index (HVI), low pour point, and keep higher base oil yield.
Below further specify the present invention with embodiment, but scope of the present invention is not limited to this specific embodiment.
Embodiment 1
To contain silica alumina ratio (SiO
2/ Al
2O
3) be that first section catalyst molecule sieve content of 212 β-1 molecular sieve is 65wt%, Pd content is 0.5wt%, the molar fraction (Si/Si+Al+P) that contains silicon is 0.21, grain size is second section catalyzer of the SAPO-1lA molecular sieve of 0.08 μ, molecular sieve content is 65wt%, Pd content is 0.5wt%, two kinds of catalyzer series connection are loaded in the small-sized hydrogenator of 200ml, the volume ratio of first section catalyzer and second section catalyzer is 1: 10, and the Middle East VGO hydrocracking tail oil that will have table 1 character enters reactor with hydrogen.In reaction conditions and the effluent＞character of 350 ℃ of cuts lists in table 2 and table 3.
Comparative example 1
Identical with the stock oil of embodiment 1, difference is only to be equipped with in the reactor the second section catalyzer that contains the SAPO-11 molecular sieve, and processing condition see Table 2, and effluent＞350 ℃ cut character sees Table 3.
Table 1 Middle East VGO hydrocracking tail oil main character density (20 ℃), kg/m
3831.4 viscosity, mm
250 ℃ of 13.8 100 ℃ of 3.902 boiling range of/s, ℃ ASTM (D1160) IBP/10% 2,52/,344 30%/50% 3,82/,403 70%/90% 430/470 95%/EBP 491/514 pour points, ℃ 39 sulphur, μ g/g 8.0 nitrogen, μ g/g 1.0P/N/A (wt%) 63.2/34.6/2.2
Table 2 reaction conditions
Embodiment 1 comparative example 1 catalyst P d/ β-1: Pd/SAPO-11A=1: 10 Pd/SAPO-11 reaction pressures, MPa 15.0 15.0H
2/ oil (volume) 800 800 temperature of reaction, ℃ 360 380LHSV, h
-10.91 1.0
In table 3 effluent＞350 ℃ of cut character
1＞350 ℃ of cut yield of embodiment 1 comparative example, wt% (to charging) 80.2 74.0 pour points, ℃-15-15 viscosity indexs 126 123
Embodiment 2
Be that with the difference of embodiment 1 raw material is Middle East VGO furfural refining oil hydrotreatment oil＞350 ℃ of cuts, feedstock property sees Table 4, in processing condition and the effluent＞and 350 ℃ of cut character see Table 5.
Table 4 Middle East VGO furfural refining oil hydrotreatment oil＞350 ℃ of cut character density (20 ℃), kg/m
3854.0 viscosity, mm
250 ℃ of 26.52 100 ℃ of 6.678 boiling range of/s, ℃ ASTMD (1160) IBP/10% 3,65/,419 30%/50% 4,43/,461 70%/90% 480/512 95%/EBP 529/549 pour points, ℃
48 sulphur, μ g/g 4.3 nitrogen, μ g/g 1.0
In table 5 processing condition and the effluent＞350 ℃ of cut character
Embodiment 2 hydrogen dividing potential drops, MPa 15.0 temperature of reaction, ℃ 370LHSV, h-1 0.91 hydrogen/oil (v) 800C
5 +Liquid yield, 96.0＞350 ℃ of cut character of wt% yield, wt% (to charging) 75 pour points, ℃-18 viscosity indexs 126
Embodiment 3
Be that with the difference of embodiment 1 raw material is a kind of cycloalkyl VGO hydrotreatment tail oil (＞350 ℃ of cut), its character sees Table 6, and processing condition and effluent＞350 ℃ cut character sees Table 7.
Table 6 cycloalkyl VGO hydrotreatment tail oil character density (20 ℃), kg/m
3871.6 boiling range, ℃ ASTMD (1160) IBP/10% 2,98/,367 30%/50% 3,97/,416 70%/90% 433/459 95%/EBP 477/505 pour points, ℃ 36 sulphur, μ g/g 21.6 nitrogen, μ g/g 2.3 wax contents, wt% 15.5 viscosity, mm
2100 ℃ of 5.023P/N/A of/s, wt% 21.5/62.0/16.3
In table 7 processing condition and the effluent＞350 ℃ of cut character
Embodiment 3 hydrogen dividing potential drops, MPa 8.0 temperature of reaction, ℃ 365LHSV, h
-10.91 hydrogen/oil (v) 800C
5 +Liquid yield, 95.8＞350 ℃ of cut character of wt% yield, wt% (to charging) 79.5 pour points, ℃-15 viscosity indexs 93
Embodiment 4
Embodiment 4 is employed β-1 molecular sieve in first section catalyzer is exchanged with 0.3NKCl solution with the difference of embodiment 1, and the volume ratio of first section catalyzer and second section catalyzer is 1: 6, and other condition is all identical with embodiment 1.Compare with embodiment 1, through K
+The acid qualitative changeization of the beta-molecular sieve (K β-1) of exchange sees Table 8.
Table 8 β-1 molecular sieve is through K
+The variation of acid matter before and after the exchange
Molecular sieve K β-1 (embodiment 4) β-1 (embodiment 1) structure B acid amount a, mmol/g 0.02 the last 0.22 B acid amount b, mmol/g 0 0.05a: it is generally acknowledged NH
3The NH of-TPD250 ℃～400 ℃ of desorptions
3Belong to structure B acid b: pyridine IR-TPD＞450 ℃ B acid amount
As seen pass through K
+β after the exchange-1 molecular sieve structure B acid and strong B acid amount all descend, thereby can reduce the lytic activity of catalyzer, improve the yield of base oil.The reaction conditions of embodiment 4 and effluent＞350 ℃ cut character sees Table 9, and stock oil is identical with embodiment 1.
In table 9 processing condition and the effluent＞350 ℃ of cut character
Embodiment 4
Catalyst P d/K β-1: Pd/SAPO-11A=1: 6
The hydrogen dividing potential drop, MPa 8.0
Temperature of reaction, ℃ 360
LHSV,h
-1 0.91
Hydrogen/oil (v) 800
C
5 +Liquid yield, wt% 96.2
＞350 ℃ of cut character
Yield, wt% (to charging) 84.0
Pour point, ℃-18
Viscosity index 121
Embodiment 5
The difference of embodiment 5 and embodiment 1 is the silica alumina ratio (SiO of employed β-2 molecular sieve in first section catalyzer
2/ Al
2O
3) be 104, after the exchange of 0.3NKCl solution, make catalyzer according to the condition identical with embodiment 1, the volume ratio of first section catalyzer and second section catalyzer is 1: 13, other condition is all identical with embodiment 1.Reaction conditions and effluent＞350 ℃ cut character sees Table 10.
In table 10 processing condition and the effluent＞350 ℃ of cut character
Embodiment 5 catalyst P d/K β-2: Pd/SAPO-11A=1: 13 hydrogen dividing potential drops, MPa 8.0 temperature of reaction, ℃ 360LHSV, h
-10.91 hydrogen/oil (v) 800C
5 +Liquid yield, 95.4＞350 ℃ of cut character of wt% yield, wt% (to charging) 59.5 pour points, ℃-9 viscosity indexs 123 embodiment 6
Embodiment 6 is that with the difference of embodiment 4 molar fraction (Si/Si+Al+P) of employed SAPO-11B molecular sieve silicon in second section catalyzer is 0.12, grain size is 0.16 μ, the volume ratio of first section catalyzer and second section catalyzer is 1: 15, and other condition is all identical with embodiment 4.Reaction conditions and effluent＞350 ℃ cut character sees Table 11.
In table 11 processing condition and the effluent＞350 ℃ of cut character
Embodiment 6 catalyst P d/K β-1: Pd/SAPO-11B=1: 15 hydrogen dividing potential drops, MPa 8.0 temperature of reaction, ℃ 370LHSV, h
-10.91 hydrogen/oil (v) 800C
5 +Liquid yield, 95.6＞350 ℃ of cut character of wt% yield, wt% (to charging) 69.0 pour points, ℃-15 viscosity indexs 121
Claims (16)
1, a kind of method of producing low pour point, base oil of high viscosity index lubricant: in the presence of hydrogen, two sections placed in-line beds in making content of wax hydrocarbon oil crude material and being contained in same reactor contact, and effluent can obtain the lubricant base oil fraction of fine intermediate oil and low pour point, high viscosity index (HVI) through fractionation.
2,, it is characterized in that described content of wax hydrocarbon oil crude material is selected from boiling point and is higher than 250 ℃ the hydrocracking tail oil or solvent-refined oil, propane deasphalting oil and slack wax, the soft wax of process hydrotreatment according to the method for claim 1.
3,, it is characterized in that described first section catalyzer contains a kind of high silica alumina ratio beta-molecular sieve and at least a VIII family noble metal component according to the method for claim 1; Wherein be used for second section catalyzer and comprise at least a VIII family noble metal component, and the mesoporous molecular sieve with shape selectivity.
4,, it is characterized in that described mesoporous molecular sieve is selected from mordenite, SAPO-11, SAPO-31, SAPO-41, ZSM-22, ZSM-23, SSZ-32 according to the method for claim 3.
5,, it is characterized in that described noble metal component is selected from platinum and/or palladium according to the method for claim 3.
6,, it is characterized in that described mesoporous molecular sieve is SAPO-11 according to the method for claim 3 or 4.
7,, it is characterized in that in the two-stage catalytic agent of the present invention that the per-cent that first section catalyzer accounts for whole catalyst volumes is 3～20% according to the method for claim 1; The per-cent that second section catalyzer accounts for whole catalyst volumes is 80～97%.
8,, it is characterized in that in the two-stage catalytic agent of the present invention that the per-cent that first section catalyzer accounts for whole catalyst volumes is 5～15% according to the method for claim 1 or 7; The per-cent that second section catalyzer accounts for whole catalyst volumes is 85～95%.
9, according to the method for claim 3, it is characterized in that first section beta-molecular sieve silica alumina ratio that catalyzer adopted greater than 70: 1, and through K
+Exchange reduces lytic activity.
10,, it is characterized in that first section beta-molecular sieve silica alumina ratio that catalyzer adopted was greater than 100: 1 according to the method for claim 9.
11,, it is characterized in that first section beta-molecular sieve silica alumina ratio that catalyzer adopted was greater than 200: 1 according to the method for claim 9.
12, according to the method for claim 9, it is characterized in that first section beta-molecular sieve that catalyzer adopted exchanges through basic metal or alkaline-earth metal ions reduces lytic activity.
13, according to the method for claim 6, the molar fraction Si/Si+Al+P that it is characterized in that described SAPO-11 molecular sieve silicon is 0.03～0.30.
14, according to the method for claim 13, the molar fraction Si/Si+Al+P that it is characterized in that described SAPO-11 molecular sieve silicon is 0.17～0.25.
15,, it is characterized in that described SAPO-11 zeolite crystal is less than 0.5 μ according to the method for claim 6.
16,, it is characterized in that described SAPO-11 zeolite crystal is 0.05～0.10 μ according to the method for claim 15.
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| CN99113304A CN1075549C (en) | 1998-12-16 | 1999-09-29 | Method for producing base oil of high viscosity index lubricant |
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|---|---|---|---|
| CN98121077.5 | 1998-12-16 | ||
| CN98121077 | 1998-12-16 | ||
| CN99113304A CN1075549C (en) | 1998-12-16 | 1999-09-29 | Method for producing base oil of high viscosity index lubricant |
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| CN1317367C (en) * | 2004-03-31 | 2007-05-23 | 中国石油化工股份有限公司 | Method for producing lubricating oil base oil |
| CN103102954A (en) * | 2011-11-10 | 2013-05-15 | 中国石油化工股份有限公司 | Production method for high-viscosity index lubricant base oil |
| CN103773485B (en) * | 2012-10-24 | 2015-11-18 | 中国石油化工股份有限公司 | A kind of production method of base oil of high viscosity index lubricant |
| CN107286982B (en) * | 2016-04-05 | 2019-03-22 | 中国石油化工股份有限公司 | A kind of preparation method of lube base oil |
| CN107286981B (en) * | 2016-04-05 | 2019-04-16 | 中国石油化工股份有限公司 | A kind of preparation method of lube base oil |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1137059A (en) * | 1995-05-19 | 1996-12-04 | 国际壳牌研究有限公司 | Process for preparation of lubricating base oils |
| CN1140199A (en) * | 1995-04-28 | 1997-01-15 | 国际壳牌研究有限公司 | Process for producing lubricating base oils |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1140199A (en) * | 1995-04-28 | 1997-01-15 | 国际壳牌研究有限公司 | Process for producing lubricating base oils |
| CN1137059A (en) * | 1995-05-19 | 1996-12-04 | 国际壳牌研究有限公司 | Process for preparation of lubricating base oils |
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