WO2000047698A1 - Kraftstoffzusammensetzung - Google Patents
Kraftstoffzusammensetzung Download PDFInfo
- Publication number
- WO2000047698A1 WO2000047698A1 PCT/EP2000/000911 EP0000911W WO0047698A1 WO 2000047698 A1 WO2000047698 A1 WO 2000047698A1 EP 0000911 W EP0000911 W EP 0000911W WO 0047698 A1 WO0047698 A1 WO 0047698A1
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- WIPO (PCT)
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- groups
- additive
- fuel composition
- petrol
- composition according
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- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L10/00—Use of additives to fuels or fires for particular purposes
- C10L10/08—Use of additives to fuels or fires for particular purposes for improving lubricity; for reducing wear
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- C10L1/00—Liquid carbonaceous fuels
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- C10L1/22—Organic compounds containing nitrogen
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- C10L1/00—Liquid carbonaceous fuels
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- C10L1/00—Liquid carbonaceous fuels
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- C10L1/192—Macromolecular compounds
- C10L1/195—Macromolecular compounds obtained by reactions involving only carbon-to-carbon unsaturated bonds
- C10L1/196—Macromolecular compounds obtained by reactions involving only carbon-to-carbon unsaturated bonds derived from monomers containing a carbon-to-carbon unsaturated bond and a carboxyl group or salts, anhydrides or esters thereof homo- or copolymers of compounds having one or more unsaturated aliphatic radicals each having one carbon bond to carbon double bond, and at least one being terminated by a carboxyl radical or of salts, anhydrides or esters thereof
- C10L1/1966—Macromolecular compounds obtained by reactions involving only carbon-to-carbon unsaturated bonds derived from monomers containing a carbon-to-carbon unsaturated bond and a carboxyl group or salts, anhydrides or esters thereof homo- or copolymers of compounds having one or more unsaturated aliphatic radicals each having one carbon bond to carbon double bond, and at least one being terminated by a carboxyl radical or of salts, anhydrides or esters thereof poly-carboxylic
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- C10L1/198—Macromolecular compounds obtained otherwise than by reactions involving only carbon-to-carbon unsaturated bonds homo- or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon to carbon double bond, and at least one being terminated by an acyloxy radical of a saturated carboxylic acid, of carbonic acid
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- C10L1/198—Macromolecular compounds obtained otherwise than by reactions involving only carbon-to-carbon unsaturated bonds homo- or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon to carbon double bond, and at least one being terminated by an acyloxy radical of a saturated carboxylic acid, of carbonic acid
- C10L1/1985—Macromolecular compounds obtained otherwise than by reactions involving only carbon-to-carbon unsaturated bonds homo- or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon to carbon double bond, and at least one being terminated by an acyloxy radical of a saturated carboxylic acid, of carbonic acid polyethers, e.g. di- polygylcols and derivatives; ethers - esters
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- C10L1/23—Organic compounds containing nitrogen containing at least one nitrogen-to-oxygen bond, e.g. nitro-compounds, nitrates, nitrites
- C10L1/231—Organic compounds containing nitrogen containing at least one nitrogen-to-oxygen bond, e.g. nitro-compounds, nitrates, nitrites nitro compounds; nitrates; nitrites
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- C10L1/236—Macromolecular compounds obtained by reactions involving only carbon-to-carbon unsaturated bonds derivatives thereof
- C10L1/2364—Macromolecular compounds obtained by reactions involving only carbon-to-carbon unsaturated bonds derivatives thereof homo- or copolymers derived from unsaturated compounds containing amide and/or imide groups
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- C10L1/238—Macromolecular compounds obtained otherwise than by reactions involving only carbon-to-carbon unsaturated bonds
- C10L1/2383—Polyamines or polyimines, or derivatives thereof (poly)amines and imines; derivatives thereof (substituted by a macromolecular group containing 30C)
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- C10L1/00—Liquid carbonaceous fuels
- C10L1/10—Liquid carbonaceous fuels containing additives
- C10L1/14—Organic compounds
- C10L1/24—Organic compounds containing sulfur, selenium and/or tellurium
- C10L1/2431—Organic compounds containing sulfur, selenium and/or tellurium sulfur bond to oxygen, e.g. sulfones, sulfoxides
- C10L1/2437—Sulfonic acids; Derivatives thereof, e.g. sulfonamides, sulfosuccinic acid esters
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- C10L1/1633—Hydrocarbons macromolecular compounds homo- or copolymers obtained by reactions only involving carbon-to carbon unsaturated bonds
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- C10L1/2222—(cyclo)aliphatic amines; polyamines (no macromolecular substituent 30C); quaternair ammonium compounds; carbamates
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- C10L1/224—Amides; Imides carboxylic acid amides, imides
Definitions
- the present invention relates to a fuel composition containing a special gasoline fuel in a larger amount and selected gasoline additives in a smaller amount.
- Carburetors and intake systems of gasoline engines are increasingly contaminated with contaminants caused by dust particles from the air, unburned hydrocarbon residues from the combustion chamber and the crankcase ventilation gases that are led into the carburetor.
- valve seat wear-inhibiting additives based on alkali or alkaline earth metal compounds have been developed.
- Modern gasoline engines require fuels with a complex property profile for trouble-free use, which can only be guaranteed in combination with appropriate gasoline additives.
- Such petrol generally consist of a complex mixture of chemical compounds and are characterized by physical quantities.
- the interaction between gasoline fuels and the corresponding additives is, however, in need of improvement in the known fuel compositions with regard to the cleaning or keeping-clean effect and the valve seat wear-inhibiting effect.
- the object of the present invention was therefore to find a more effective gasoline / gasoline / gasoline additive composition.
- a fuel composition which in a larger amount contains a petrol with an aromatic content of at most 42 vol.% And a sulfur content of at most 150 ppm by weight, and in a smaller amount at least one petrol additive with detergent effect or with valve seat wear-inhibiting effect, this gasoline additive containing at least one hydrophobic hydrocarbon residue with a number average molecular weight (M N ) of 85 to 20,000 and at least one polar grouping selected
- At least one nitrogen atom having basic natural sheep has hydroxyl groups, mono- or polyamino min ⁇ en, or by carbamate groups,
- the aromatic content of the petrol is preferably at most 40% by volume, in particular at most 38% by volume. Preferred ranges for the aromatic content are 20 to 42% by volume, in particular 25 to 40% by volume.
- the sulfur content of the petrol is preferably at most 100 ppm by weight, in particular at most 50 ppm by weight. Preferred ranges for the sulfur content are 0.5 to 150 ppm by weight, in particular 1 to 100 ppm by weight.
- the petrol has an olefin content of at most 21% by volume, preferably at most 18% by volume, in particular at most 10% by volume. Preferred ranges for the olefin content are 6 to 21% by volume, in particular 7 to 18% by volume.
- the petrol has a benzene content of at most 1.0% by volume, in particular at most 0.9% by volume.
- Preferred ranges for the benzene content are 0.5 to 1.0% by volume, in particular 0.6 to 0.9% by volume.
- the petrol has an oxygen content of at most 2.7% by weight, preferably from 0.1 to 2.7% by weight, especially from 1.0 to 2.7% by weight. , in particular from 1.2 to 2.0% by weight.
- a petrol which at the same time has an aromatic content of at most 38 vol.%, An olefin content of at most 21 vol.%, A sulfur content of at most 50 ppm by weight, a benzene content of at most 1.0 vol.% And one Oxygen content from 1.0 to 2.7% by weight.
- the alcohol and ether content in petrol is usually relatively low. Typical maximum contents are 3 vol.% For methanol, 5 vol.% For ethanol, 10 vol.% For isopropanol, for tert. -Butanol 7 vol .-%, for isobutanol 10 vol .-% and for ethers with 5 or more carbon atoms in the molecule 15 vol .-%.
- the summer vapor pressure of petrol is usually a maximum of 70 kPa, especially 60 kPa (each at 37 ° C).
- the research octane number ("RON") of the petrol is usually 90 to 100.
- a common range for the corresponding engine octane number (“MOZ”) is 80 to 90.
- the specifications mentioned are determined using customary methods (DIN EN 228).
- the hydrophobic hydrocarbon residue in the petrol additives which ensures sufficient solubility in the fuel, has a number average molecular weight (M N ) from 85 to 20,000, in particular from 113 to 10,000, especially from 300 to 5,000.
- M N number average molecular weight
- Such additives based on highly reactive polyisobutene, which from the polyisobutene, which can contain up to 20% by weight of n-butene units, by hydroformylation and reductive amination with ammonia, monoamines or polyamines such as Dimethylaminopropylamine, ethylenediamine, diethylenetriamine, triethylenetetramine or tetraethylene pentamine can be produced, are known in particular from EP-A 244 616.
- reaction products are usually mixtures of pure nitropolyisobutanes (e.g. ⁇ , ⁇ -dinitropolyisobutane) and mixed hydroxynitropolyisobutanes
- Additives containing carboxyl groups or their alkali metal or alkaline earth metal salts (d) are preferably copolymers of C 2 -C 4 o-olefins with maleic anhydride with a total molar mass of 500 to 20,000, the carboxyl groups of which are wholly or partly to the alkali metal or Alkaline earth metal salts and a remainder of the carboxyl groups are reacted with alcohols or amines.
- Such additives are known in particular from EP-A 307 815.
- Such additives mainly serve to prevent valve seat wear and, as described in WO-A 87/01126, can advantageously be used in combination with conventional fuel detergents such as poly (iso) butenamines or polyetheramines.
- Additives containing sulfonic acid groups or their alkali metal or alkaline earth metal salts (s) are preferably alkali metal or alkaline earth metal salts of an alkyl sulfosuccinic acid ester, as described in particular in EP-A 639 632.
- Such additives mainly serve to prevent valve seat wear and can advantageously be used in combination with conventional fuel detergents such as poly (iso) butenamines or polyetheramines.
- Additives containing polyoxy-C 2 to C 4 -alkylene groupings (f) are preferably polyethers or polyether amines which are obtained by reacting C to C 6 o-alkanols, C 6 to C 30 alkanediols, mono- or di-C 2 -C 30 alkylamines, C ⁇ -C 30 alkylcyclohexanols or C 1 -C 30 alkylphenols with 1 to 30 mol of ethylene oxide and / or
- Propylene oxide and / or butylene oxide per hydroxyl group or amino group and, in the case of the polyetheramines, can be obtained by subsequent reductive amination with ammonia, monoamines or polyamines.
- Such products are described in particular in EP-A 310 875, EP-A 356 725, EP-A 700 985 and US-A 4 877 416.
- polyethers such products also have carrier oil properties. Typical examples of this are tridecanol or isotridecanol butoxylates, isononylphenol butoxylates and polyisobutenol butoxylates and propoxylates as well as the corresponding reaction products with ammonia.
- Additives containing carboxylic acid ester groups (g) are preferably esters of mono-, di- or tricarboxylic acids with long-chain alkanols or polyols, in particular those with a minimum viscosity of 2 mm 2 / s at 100 ° C., as described in particular in
- Aliphatic or aromatic acids can be used as mono-, di- or tricarboxylic acids, and long-chain representatives with, for example, 6 to 24 carbon atoms are particularly suitable as ester alcohols or polyols.
- Typical representatives of the esters are adipates, phthalates, isophthalates, terephthalates and trimellitates of iso-octanol, iso-nonanol, iso-decanol and iso-tridecanol.
- Such products also have carrier oil properties.
- Derivatives with aliphatic polyamines such as ethylene diamine, diethylene triamine, triethylene tetramine or tetraethylene pentamine are of particular interest.
- Such gasoline fuel additives are described in particular in US Pat. No. 4,849,572.
- Groupings (i) containing additives produced by Mannich reaction of substituted phenols with aldehydes and mono- or polyamines are preferably reaction products of polyisobutene-substituted phenols with formaldehyde and mono- or polyamines such as ethylenediamine, diethylenetriamine, triethylenetetramine, tetraethylenepentamine or dirnethylaminopropylamine.
- Such “polyisobutene Mannich bases” are described in particular in EP-A 831 141.
- the fuel composition according to the invention can also contain other conventional components and additives.
- solvents or diluents there are aliphatic and aromatic hydrocarbons, e.g. Solvent Naphtha.
- corrosion inhibitors for example based on ammonium salts of organic carboxylic acids which tend to form films, or of heterocyclic aromatics in the case of non-ferrous metal corrosion protection, antioxidants or stabilizers, for example based on amines such as p-phenylenediamine, dicyclohexylamine or derivatives thereof or phenols such as 2 , 4-di- tert. -butylphenol or 3, 5 -ditert.
- demulsifiers demulsifiers, antistatic agents, metallocenes such as ferrocene or methylcyclopentadienylmanganese tricarbonyl, lubricity improvers (lubricity additives) such as certain fatty acids, alkenylsuccinic acid esters, bis (hydroxyalkyl) fatty amines, ricinoleic acids and hydroxyacetamides or hydroxyacetamides ). Sometimes amines are added to lower the pH of the fuel.
- Combinations of the gasoline described with a mixture of gasoline additives with the polar grouping (f) and corrosion inhibitors and / or lubricity improvers based on carboxylic acids or fatty acids, which may be present as monomeric and / or dimeric species, are also used for the fuel composition according to the invention , into consideration.
- Typical mixtures of this type contain polyisobutene amines in combination with alkanol-started polyethers such as tridecanol or isotridecanol butoxylates or propoxylates, poly- isobutenamines in combination with alkanol-started polyether amines such as tridecanol or isotridecanol butoxylate-ammonia reaction products and alkanol-started polyether amines such as tridecanol or isotridecaolbutoxyla-ammonia reaction products in combination with alkanol-started polyethers or isotatenate propanol-together with trisecenate-ethoxylates - trideceno-benzo Lubricant - improving the quality.
- alkanol-started polyethers such as tridecanol or isotridecanol butoxylates or propoxylates
- gasoline fuel additives with the polar groupings (a) to (i) and the other components mentioned are metered into the gasoline fuel and develop their effect there.
- the components or additives can be added to the petrol individually or as a previously prepared concentrate (“additive package”).
- the petrol additives mentioned with the polar groupings (a) to (i) are usually added to the petrol in an amount of 1 to 5000 ppm by weight, in particular 5 to 3000 ppm by weight, especially 10 to 1000 ppm by weight .
- the other components and additives mentioned are added, if desired, in amounts customary for this.
- the same cleaning or keeping-in or valve seat wear-inhibiting effect can be achieved as in conventional fuel compositions of the prior art.
- the same amounts of detergent or valve seat wear-inhibiting agent in the fuel composition according to the invention compared to conventional fuel compositions, there is a significantly better cleaning or cleaning effect or valve seat wear-inhibiting effect.
- the fuel composition according to the invention also has advantages in that fewer deposits are formed in the combustion chamber of the gasoline engine and that less additive is introduced into the engine oil via the fuel dilution.
- Example 10 500 mg of a commercial additive composition for petrol, containing 60% by weight of the same polyisobutenamine as in Example 1 and mineral carrier oil and corrosion protection, each in the usual amounts (Keropur® 3233 from BASF Aktiengesellschaft), were made in 1 kg of OKI Table 1 solved.
- Example 10 500 mg of a commercial additive composition for petrol, containing 60% by weight of the same polyisobutenamine as in Example 1 and mineral carrier oil and corrosion protection, each in the usual amounts (Keropur® 3233 from BASF Aktiengesellschaft), were made in 1 kg of OKI Table 1 solved.
- Example 10 500 mg of a commercial additive composition for petrol, containing 60% by weight of the same polyisobutenamine as in Example 1 and mineral carrier oil and corrosion protection, each in the usual amounts (Keropur® 3233 from BASF Aktiengesellschaft), were made in 1 kg of OKI Table 1 solved.
- Example 10 500 mg of a commercial additive composition for petrol, containing 60% by weight of the same polyisobutenamine as in Example 1 and mineral carrier oil and corrosion protection
- Example 2 Gasoline according to Example 1 was tested for its suitability for intake system cleanliness. This was done with the help of engine tests that were carried out in test bench tests with a Mercedes-Benz engine in accordance with CEC F-05-A-93. As expected, the intake valve deposits were significantly reduced compared to the non-additive base value according to Table 2 below.
- Example 2 Gasoline according to Example 2 was tested for its suitability for intake system cleanliness. This was done with the help of engine tests that were carried out in test bench tests with a Mercedes-Benz engine CEC F-05-A-93. As expected, the intake valve deposits were significantly reduced compared to the non-additive base value according to Table 2 below. Surprisingly, it was found that, compared to Example 13, the inlet valves were kept completely clean with the same amount of fuel additive.
- Example 3 Gasoline according to Example 3 was tested for its suitability for intake system cleanliness. This was done with the help of engine tests, which were carried out in test bench tests with a Mercedes Benz engine CEC F-05-A-93 were carried out. As expected, the intake valve deposits were significantly reduced compared to the non-additive base value according to Table 2 below.
- Example 4 Gasoline according to Example 4 was tested for its suitability for intake system cleanliness. This was done with the help of engine tests that were carried out in test bench tests with a Mercedes-Benz engine CEC F-05-A-93. As expected, the intake valve deposits were significantly reduced compared to the non-additive base value according to Table 2 below. Surprisingly, it was found that, in comparison with Example 15, the intake valves are kept practically completely clean with the same amount of fuel additive.
- Example 5 Gasoline according to Example 5 was tested for its suitability for intake system cleanliness. This was done with the help of engine tests that were carried out in test bench tests with a Mercedes-Benz engine CEC F-05-A-93. As expected, the intake valve deposits were significantly reduced compared to the non-additive base value according to Table 2 below.
- Example 6 Gasoline according to Example 6 was tested for its suitability for intake system cleanliness. This was done with the help of engine tests that were carried out in test bench tests with a Mercedes-Benz engine CEC F-05-A-93. As expected, the intake valve deposits were significantly reduced compared to the non-additive base value according to Table 2 below. Surprisingly, it was found that, in comparison to Example 17, the intake valves are kept practically completely clean with the same amount of fuel additive.
- Example 7 Gasoline according to Example 7 was tested for its suitability for intake system cleanliness. This was done with the help of engine tests that were carried out in test bench tests with a Mercedes-Benz engine CEC F-05-A-93. As expected, the intake valve deposits were not compared to that additive base value according to Table 2 below significantly reduced.
- Example 8 Gasoline according to Example 8 was tested for its suitability for intake system cleanliness. This was done with the help of engine tests that were carried out in test bench tests with a Mercedes-Benz engine CEC F-05-A-93. As expected, the intake valve deposits were significantly reduced compared to the non-additive base value according to Table 2 below. Surprisingly, it was found that significantly less fuel additive is required compared to Example 19 to keep the intake valves clean on the same order of magnitude.
- Example 9 Gasoline according to Example 9 was tested for its suitability for intake system cleanliness. This was done with the help of engine tests that were carried out in test bench tests with a Mercedes-Benz engine CEC F-05-A-93. As expected, the intake valve deposits were significantly reduced compared to the non-additive base value according to Table 2 below.
- Example 10 Gasoline according to Example 10 was examined for its suitability for intake system cleanliness. This was done with the aid of engine tests which were carried out in bench tests with a Mer ⁇ cedes-Benz engine CEC F-05-A-93rd As expected, the intake valve deposits were significantly reduced compared to the non-additive base value according to Table 2 below. Surprisingly, it was found that, in comparison to Example 21, the intake valve was kept much cleaner with the same amount of fuel additive.
- Gasoline according to Example 11 was tested for its suitability for intake system cleanliness. This was done with the help of engine tests that were carried out in test bench tests with a Mercedes-Benz engine CEC F-05-A-93. The intake valve deposits were not expected as compared to additive base value according to Table 2 below significantly reduced.
- Example 12 Gasoline according to Example 12 was tested for its suitability for intake system cleanliness. This was done with the help of engine tests that were carried out in test bench tests with a Mercedes-Benz engine CEC F-05-A-93. As expected, the intake valve deposits were significantly reduced compared to the non-additive base value according to Table 2 below. Surprisingly, it was found that, in comparison to Example 23, the intake valves were kept much cleaner with the same amount of fuel additive.
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Abstract
Description
Claims
Priority Applications (12)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
AU34220/00A AU766424B2 (en) | 1999-02-09 | 2000-02-05 | Fuel composition |
CA002359723A CA2359723A1 (en) | 1999-02-09 | 2000-02-05 | Fuel composition |
NZ513306A NZ513306A (en) | 1999-02-09 | 2000-02-05 | Fuel composition |
IL14437500A IL144375A (en) | 1999-02-09 | 2000-02-05 | A vehicle fuel composition containing polymers as additives |
BR0008087-0A BR0008087A (pt) | 1999-02-09 | 2000-02-05 | Composição combustìvel |
EP00912452A EP1155102A1 (de) | 1999-02-09 | 2000-02-05 | Kraftstoffzusammensetzung |
SK1085-2001A SK10852001A3 (sk) | 1999-02-09 | 2000-02-05 | Palivová kompozícia |
PL349860A PL191309B1 (pl) | 1999-02-09 | 2000-02-05 | Kompozycja paliwowa |
EEP200100420A EE200100420A (et) | 1999-02-09 | 2000-02-05 | Kütusekoostis |
JP2000598599A JP2002536531A (ja) | 1999-02-09 | 2000-02-05 | 燃料組成物 |
NO20013864A NO20013864D0 (no) | 1999-02-09 | 2001-08-08 | Brenselsblanding |
HR20010661A HRP20010661A2 (en) | 1999-02-09 | 2001-09-07 | Fuel composition |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE19905211.5 | 1999-02-09 | ||
DE19905211A DE19905211A1 (de) | 1999-02-09 | 1999-02-09 | Kraftstoffzusammensetzung |
Related Child Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
US10/953,609 Continuation US20050044779A1 (en) | 1999-02-09 | 2004-09-30 | Fuel composition |
Publications (1)
Publication Number | Publication Date |
---|---|
WO2000047698A1 true WO2000047698A1 (de) | 2000-08-17 |
Family
ID=7896865
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
PCT/EP2000/000911 WO2000047698A1 (de) | 1999-02-09 | 2000-02-05 | Kraftstoffzusammensetzung |
Country Status (22)
Country | Link |
---|---|
EP (3) | EP1277828A3 (de) |
JP (1) | JP2002536531A (de) |
KR (1) | KR100663774B1 (de) |
AR (1) | AR022534A1 (de) |
AU (1) | AU766424B2 (de) |
BR (1) | BR0008087A (de) |
CA (1) | CA2359723A1 (de) |
CZ (1) | CZ20012854A3 (de) |
DE (1) | DE19905211A1 (de) |
EE (1) | EE200100420A (de) |
HR (1) | HRP20010661A2 (de) |
HU (1) | HUP0200270A3 (de) |
IL (1) | IL144375A (de) |
MY (1) | MY121511A (de) |
NO (1) | NO20013864D0 (de) |
NZ (1) | NZ513306A (de) |
PL (1) | PL191309B1 (de) |
RU (1) | RU2238300C2 (de) |
SK (1) | SK10852001A3 (de) |
TR (1) | TR200102283T2 (de) |
WO (1) | WO2000047698A1 (de) |
ZA (1) | ZA200107409B (de) |
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Also Published As
Publication number | Publication date |
---|---|
HUP0200270A3 (en) | 2003-08-28 |
EP1155102A1 (de) | 2001-11-21 |
IL144375A0 (en) | 2002-05-23 |
AR022534A1 (es) | 2002-09-04 |
EP1612257A2 (de) | 2006-01-04 |
NZ513306A (en) | 2003-01-31 |
KR100663774B1 (ko) | 2007-01-03 |
BR0008087A (pt) | 2001-11-06 |
CZ20012854A3 (cs) | 2002-05-15 |
NO20013864L (no) | 2001-08-08 |
HRP20010661A2 (en) | 2003-04-30 |
SK10852001A3 (sk) | 2002-06-04 |
DE19905211A1 (de) | 2000-08-10 |
KR20010111491A (ko) | 2001-12-19 |
MY121511A (en) | 2006-01-28 |
EE200100420A (et) | 2002-12-16 |
PL191309B1 (pl) | 2006-04-28 |
JP2002536531A (ja) | 2002-10-29 |
ZA200107409B (en) | 2003-01-29 |
AU766424B2 (en) | 2003-10-16 |
PL349860A1 (en) | 2002-09-23 |
EP1277828A3 (de) | 2003-07-02 |
EP1277828A2 (de) | 2003-01-22 |
HUP0200270A2 (hu) | 2002-05-29 |
AU3422000A (en) | 2000-08-29 |
NO20013864D0 (no) | 2001-08-08 |
IL144375A (en) | 2004-08-31 |
RU2238300C2 (ru) | 2004-10-20 |
CA2359723A1 (en) | 2000-08-17 |
TR200102283T2 (tr) | 2001-12-21 |
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