EP0932483A1 - Wässrige betontrennmittel - Google Patents
Wässrige betontrennmittelInfo
- Publication number
- EP0932483A1 EP0932483A1 EP97944851A EP97944851A EP0932483A1 EP 0932483 A1 EP0932483 A1 EP 0932483A1 EP 97944851 A EP97944851 A EP 97944851A EP 97944851 A EP97944851 A EP 97944851A EP 0932483 A1 EP0932483 A1 EP 0932483A1
- Authority
- EP
- European Patent Office
- Prior art keywords
- alkyl
- contain
- fatty alcohols
- aqueous
- agents
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B28—WORKING CEMENT, CLAY, OR STONE
- B28B—SHAPING CLAY OR OTHER CERAMIC COMPOSITIONS; SHAPING SLAG; SHAPING MIXTURES CONTAINING CEMENTITIOUS MATERIAL, e.g. PLASTER
- B28B7/00—Moulds; Cores; Mandrels
- B28B7/38—Treating surfaces of moulds, cores, or mandrels to prevent sticking
- B28B7/384—Treating agents
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
- C10M129/00—Lubricating compositions characterised by the additive being an organic non-macromolecular compound containing oxygen
- C10M129/02—Lubricating compositions characterised by the additive being an organic non-macromolecular compound containing oxygen having a carbon chain of less than 30 atoms
- C10M129/04—Hydroxy compounds
- C10M129/06—Hydroxy compounds having hydroxy groups bound to acyclic or cycloaliphatic carbon atoms
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
- C10M145/00—Lubricating compositions characterised by the additive being a macromolecular compound containing oxygen
- C10M145/40—Polysaccharides, e.g. cellulose
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
- C10M173/00—Lubricating compositions containing more than 10% water
- C10M173/02—Lubricating compositions containing more than 10% water not containing mineral or fatty oils
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
- C10M2207/00—Organic non-macromolecular hydrocarbon compounds containing hydrogen, carbon and oxygen as ingredients in lubricant compositions
- C10M2207/02—Hydroxy compounds
- C10M2207/021—Hydroxy compounds having hydroxy groups bound to acyclic or cycloaliphatic carbon atoms
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
- C10M2209/00—Organic macromolecular compounds containing oxygen as ingredients in lubricant compositions
- C10M2209/12—Polysaccharides, e.g. cellulose, biopolymers
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
- C10N2040/00—Specified use or application for which the lubricating composition is intended
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
- C10N2040/00—Specified use or application for which the lubricating composition is intended
- C10N2040/30—Refrigerators lubricants or compressors lubricants
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
- C10N2040/00—Specified use or application for which the lubricating composition is intended
- C10N2040/32—Wires, ropes or cables lubricants
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
- C10N2040/00—Specified use or application for which the lubricating composition is intended
- C10N2040/34—Lubricating-sealants
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
- C10N2040/00—Specified use or application for which the lubricating composition is intended
- C10N2040/36—Release agents or mold release agents
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
- C10N2040/00—Specified use or application for which the lubricating composition is intended
- C10N2040/38—Conveyors or chain belts
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
- C10N2040/00—Specified use or application for which the lubricating composition is intended
- C10N2040/40—Generators or electric motors in oil or gas winning field
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
- C10N2040/00—Specified use or application for which the lubricating composition is intended
- C10N2040/42—Flashing oils or marking oils
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
- C10N2040/00—Specified use or application for which the lubricating composition is intended
- C10N2040/44—Super vacuum or supercritical use
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
- C10N2040/00—Specified use or application for which the lubricating composition is intended
- C10N2040/50—Medical uses
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10N—INDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
- C10N2050/00—Form in which the lubricant is applied to the material being lubricated
- C10N2050/01—Emulsions, colloids, or micelles
Definitions
- the invention relates to aqueous concrete release agents based on selected oil bodies and emulsifiers, a process for their preparation and the use of the mixtures of selected oil bodies and emulsifiers for the production of aqueous concrete release agents.
- P. 319f. They are applied to the formwork before the fresh concrete is poured in and are intended to reduce the adhesion between the concrete and the formwork and to avoid damage to the concrete surface and the formwork.
- the aim is to increase the number of technically possible uses of the formwork material.
- the release agents generally contain an oil component, as well as various additives, e.g. Antirust agents, antioxidants, antipore agents, preservatives, wetting agents, adhesives and emulsifiers.
- various substance classes or their mixtures are used as the oil component, e.g. Mineral oils or white oils, waxes, triglycerides based on vegetable or animal oils or fats or fat derivatives.
- the use of the concrete release agent in the form of an aqueous emulsion is particularly advantageous.
- the release agents generally contain emulsifiers such as soaps, ethoxylated fatty acids and ethoxylated alkylphenols or petroleum sulfonates in amounts of about 10 to 30% by weight, based on the oil component.
- emulsifiers such as soaps, ethoxylated fatty acids and ethoxylated alkylphenols or petroleum sulfonates in amounts of about 10 to 30% by weight, based on the oil component.
- the release agents are usually not delivered to the point of use as an emulsion, but in the form of a concentrate which is diluted immediately before use.
- the release agents used today have various disadvantages.
- Mineral oils or white oils are insufficiently biodegradable as an oil component.
- Triglycerides on a native basis for example beet oil, are readily biodegradable, but they have relatively high viscosities which are unfavorable for use on.
- saponification of the oil by alkaline components of the concrete can lead to the precipitation of calcium soaps, the so-called sanding, which can cause adhesion problems when the concrete is further processed.
- Fatty acid esters show similar behavior. It has already been proposed to remedy the fatty alcohol production by using distillation residues, but it has been shown that these compounds can only be used in part as an oil component, as described, for example, in D-A5 290 439.
- the oil component used here is 80 to 90% by weight of mineral oil, to which 4 to 10% by weight of a mixture of saturated and unsaturated wax esters with 32 to 36 carbon atoms, saturated and unsaturated fatty alcohols with 24 to 32 carbon atoms and hydrocarbon are added.
- the wax esters present in the mixture can moreover saponify and thus trigger the liability problems described above.
- WO £ 5/18704 (Henkel) concrete release agents which contain unsaturated fatty alcohols or Guerbet alcohols as oil components and nonionic surfactants of the alkylene oxide addition adduct type to suitable H-acidic compounds as emulsifiers.
- European patent application EP-A 0 561 465 discloses mold release agents which contain esters of sterically hindered, polyfunctional alcohols as mandatory components. The concomitant use of monofunk nonalcohols is described as a way of reducing the amount of emulsifier.
- British patent application GB-A 1 294 038 relates to a process for the production of concrete release agents, in which monofunctional alcohols are used in combination with cationic surfactants.
- the emulsifiers used for the production of aqueous emulsions are also not without problems from an application point of view. Until now, relatively large amounts of emulsifier had to be used to prepare the emulsions, but this has a negative effect on the rain resistance of the release agents. In addition, if the emulsifier content is high, re-emulsification can take place at the interface with the alkaline cement, with part of the release agent penetrating into the surface of the concrete. These residues of release agent can later lead to the problems already mentioned with the adhesion of paints or plasters.
- the invention relates to aqueous concrete release agents containing (a) unsaturated fatty alcohols and (b) alkyl and / or alkenyl oligoglycosides.
- the agents according to the invention have an improved rheology and storage stability compared to the prior art, especially in the range of low temperatures.
- the preparations are saponification-stable, free of shipping, show a strong network effect and also adhere to a wide variety of formwork materials.
- Another advantage is that the new agents are ecologically harmless and can therefore be classified in water hazard class 0
- unsaturated fatty alcohols which preferably follow the formula (I) are used as the oil component (a),
- R 1 represents a completely or predominantly unsaturated hydrocarbon radical having 6 to 22, preferably 12 to 18, carbon atoms.
- Typical examples are palmoleyl alcohol, oleyl alcohol, elaidyl alcohol, petroselinyl alcohol, linolyl alcohol, linolenyl alcohol, gadoleyl alcohol and erucyl alcohol as well as their technical mixtures, such as those obtained in the high pressure hydrogenation of technical fatty acid methyl ester fractions to obtain the double bonds.
- Typical methyl ester mixtures which are suitable as starting materials for the production of the unsaturated fatty alcohols are those which are derived from beef tallow, old and new breed sunflower oil, old and new breed beet oil, linseed oil, peanut oil and the like.
- too Methyl esters based on predominantly saturated fats and oils, such as palm oil, palm kernel oil and / or coconut oil, are used, provided that the products are subsequently concentrated accordingly, as described, for example, in documents DE-C2 43 38 974, DE-A1 43 35 781, DE -A1 44 25 180 and DE-C1 44 22 858 (Henkel) is described.
- the agents usually contain unsaturated fatty alcohols which have an iodine number in the range from 40 to 200, preferably 50 to 150 and in particular 70 to 100.
- the unsaturated fatty alcohols are generally present in amounts of 10 to 50, preferably 20 to 40% by weight, based on the composition.
- Alkyl and alkenyl oligoglycosides which are suitable as emulsifier components (b) are known nonionic surfactants which follow the formula (I)
- R 1 is an alkyl and / or alkenyl radical having 4 to 22 carbon atoms
- G is a sugar radical having 5 or 6 carbon atoms
- p is a number from 1 to 10.
- the alkyl and / or alkenyl oligoglycosides can be derived from aldoses or ketoses with 5 or 6 carbon atoms, preferably glucose.
- the preferred alkyl and / or alkenyl oligoglycosides are thus alkyl and / or alkenyl oligoglucosides.
- the index number p in the general formula (I) indicates the degree of oligomerization (DP), i.e. H. the distribution of mono- and oligoglycosides is present and stands for a number between 1 and 10.
- alkyl oligoglycoside is an analytically calculated quantity, which usually represents a fractional number.
- Alkyl and / or alkenyl oligoglycosides with an average degree of oligomerization p of 1.1 to 3.0 are preferably used. From an application point of view, preference is given to those alkyl and / or alkenyl oligoglycosides whose degree of oligomerization is less than 1.7 and in particular between 1.2 and 1.4.
- the alkyl or alkenyl radical R ' can be derived from primary alcohols having 4 to 11, preferably 8 to 10, carbon atoms. Typical examples are butanol, capro alcohol, caprylic alcohol, capric alcohol and undecyl alcohol and their technical mixtures, such as are obtained, for example, in the hydrogenation of technical fatty acid methyl esters or in the course of the hydrogenation of aldehydes from Roelen's oxosynthesis.
- the alkyl or alkenyl radical R 'can also be derived from primary alcohols having 12 to 22, preferably 12 to 14, carbon atoms.
- Typical examples are lauryl alcohol, myristyl alcohol, cetyl alcohol, palmoleyl alcohol, stearyl alcohol, isostearyl alcohol, oleyl alcohol, elaidyl alcohol, petroselinyl alcohol, arachyl alcohol, gadoleyl alcohol, behenyl alcohol, erucyl alcohol, brassidyl alcohol and the like technical mixtures which can be obtained as described above.
- Alkyl oligoglucosides based on hardened coconut alcohol with a DP of 1 to 3 are preferred.
- the alkyl and / or alkenyl oligoglycosides are usually present in amounts of 0.2 to 5, preferably 0.5 to 2% by weight. based on the composition - containing, while the means such as an aqueous component in the calibration Be r of 50 to 90, in particular 50 - 80 comprise, and preferably 60 to 70 wt .-%.
- the agents according to the invention can contain minor auxiliaries and additives such as e.g. Contain anti-corrosion agents, antioxidants, antipore agents, preservatives, wetting agents, adhesives and the like.
- the proportion of these substances, based on the composition, is usually in the range from 0.1 to 15 and preferably 0.1 to 5% by weight.
- Another object of the invention relates to a process for the preparation of aqueous concrete release agents, in which an aqueous premix is first prepared from the oil body and the emulsifier with moderate stirring and then subsequently in a manner known per se, for example in an Ultraturrax, a Supraton or another high-pressure or gear rim homogenizer, homogenized into a fine-particle emulsion.
- the release agents can be applied to the formwork surfaces in pure form or in the form of their emulsion by spraying, spraying, brushing, brushing or brushing.
- the low-viscosity emulsions are so stable that they can be sprayed without problems.
- Highly viscous pastes can also be applied with a spatula.
- Another object of the invention therefore relates to the use of mixtures of (a) unsaturated fatty alcohols and (b) alkyl and / or alkenyl oligoglycosides for the production of concrete release agents which are used for steel, plastic or wooden formwork in concrete construction. Examples
- the viscosity of the emulsions was determined using the Brookfield method in an R VT viscometer (20 * C, spindle 4, 10 rpm). The stability of the emulsions was assessed after storage over a period of 4 weeks at 5 ° C.
- the performance properties of the emulsions are summarized in Table 1.
- Mixture R1 is according to the invention, mixtures R2 to R6 are used for comparison. It can be seen that the viscosity is low and cold-stable concrete release agents can only be obtained using the combination of selected oil component and emulsifier according to the invention.
Abstract
Description
Claims
Applications Claiming Priority (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE19637841 | 1996-09-17 | ||
DE19637841A DE19637841A1 (de) | 1996-09-17 | 1996-09-17 | Wäßrige Betontrennmittel |
PCT/EP1997/004870 WO1998012032A1 (de) | 1996-09-17 | 1997-09-08 | Wässrige betontrennmittel |
Publications (2)
Publication Number | Publication Date |
---|---|
EP0932483A1 true EP0932483A1 (de) | 1999-08-04 |
EP0932483B1 EP0932483B1 (de) | 2003-12-03 |
Family
ID=7805874
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP97944851A Expired - Lifetime EP0932483B1 (de) | 1996-09-17 | 1997-09-08 | Wässrige betontrennmittel |
Country Status (5)
Country | Link |
---|---|
US (1) | US6274192B1 (de) |
EP (1) | EP0932483B1 (de) |
DE (2) | DE19637841A1 (de) |
NO (1) | NO991274D0 (de) |
WO (1) | WO1998012032A1 (de) |
Families Citing this family (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE19723604A1 (de) * | 1997-06-05 | 1998-12-10 | Henkel Kgaa | Wäßrige Betontrennmittel |
Family Cites Families (19)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE290439C (de) | ||||
GB1294038A (en) | 1969-06-26 | 1972-10-25 | Paul Low Beer | Mould release agent |
USH444H (en) * | 1985-05-20 | 1988-03-01 | A. E. Staley Manufacturing Company | Process for making molded articles with mold release agents |
DE3723826A1 (de) | 1987-07-18 | 1989-01-26 | Henkel Kgaa | Verfahren zur herstellung von alkylglykosiden |
US5576425A (en) | 1988-10-05 | 1996-11-19 | Henkel Kommanditgesellschaft Auf Aktien | Process for the direct production of alkyl glycosides |
DE3833780A1 (de) | 1988-10-05 | 1990-04-12 | Henkel Kgaa | Verfahren zur direkten herstellung von alkylglykosiden |
DE4033928A1 (de) * | 1990-10-25 | 1992-04-30 | Henkel Kgaa | Oel-in-wasser-emulsionen |
FR2668080B1 (fr) * | 1990-10-17 | 1993-08-13 | Seppic Sa | Compositions auto-emulsionnables a base d'alcools gras, leur procede de preparation et leur utilisation pour la realisation d'emulsions. |
EP0773091A3 (de) | 1992-03-20 | 1998-04-01 | Unichema Chemie B.V. | Formtrennzusammensetzung |
DE4306796A1 (de) * | 1993-03-04 | 1994-09-08 | Wacker Chemie Gmbh | Emulsionen polare Gruppen enthaltender Organopolysiloxane mit Alkylpolyglykosiden als Emulgatoren |
DE4317089A1 (de) * | 1993-05-21 | 1994-11-24 | Henkel Kgaa | Nichtionische Emulgatoren |
DE4335781C2 (de) | 1993-10-20 | 1998-02-19 | Henkel Kgaa | Fettalkohole auf pflanzlicher Basis und Verfahren zu Ihrer Herstellung |
DE4338974C2 (de) | 1993-11-15 | 1996-12-05 | Henkel Kgaa | Verfahren zur Herstellung von Fettalkoholen mit verbesserter Produktqualität |
EP0738205B1 (de) | 1994-01-10 | 1998-03-11 | Henkel Kommanditgesellschaft auf Aktien | Formtrennmittel für hydraulische bindemittel |
DE4400272A1 (de) * | 1994-01-10 | 1995-07-13 | Henkel Kgaa | Betontrennmittel |
DE4425180C2 (de) | 1994-07-16 | 1997-05-07 | Henkel Kgaa | Verfahren zur Herstellung ungesättigter Fettalkohole oder deren veresterte, alkoxylierte und/oder sulfatierte Derivate mit verbessertem Kälteverhalten |
DE19529907A1 (de) * | 1995-08-15 | 1997-02-20 | Henkel Kgaa | Feinteilige Emulsionen enthaltend Zuckertenside |
DE29520746U1 (de) * | 1995-11-15 | 1996-04-04 | Henkel Kgaa | Emulgatoren |
DE19607977A1 (de) * | 1996-03-01 | 1997-09-04 | Henkel Kgaa | Verwendung von Emulgatormischungen |
-
1996
- 1996-09-17 DE DE19637841A patent/DE19637841A1/de not_active Ceased
-
1997
- 1997-09-08 WO PCT/EP1997/004870 patent/WO1998012032A1/de active IP Right Grant
- 1997-09-08 DE DE59711077T patent/DE59711077D1/de not_active Expired - Lifetime
- 1997-09-08 US US09/254,620 patent/US6274192B1/en not_active Expired - Fee Related
- 1997-09-08 EP EP97944851A patent/EP0932483B1/de not_active Expired - Lifetime
-
1999
- 1999-03-16 NO NO991274A patent/NO991274D0/no not_active Application Discontinuation
Non-Patent Citations (1)
Title |
---|
See references of WO9812032A1 * |
Also Published As
Publication number | Publication date |
---|---|
EP0932483B1 (de) | 2003-12-03 |
NO991274L (no) | 1999-03-16 |
NO991274D0 (no) | 1999-03-16 |
DE19637841A1 (de) | 1998-03-26 |
DE59711077D1 (de) | 2004-01-15 |
WO1998012032A1 (de) | 1998-03-26 |
US6274192B1 (en) | 2001-08-14 |
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