EP0773281A2 - Préparations pour refrigerants Inbrifiants stabilisées - Google Patents

Préparations pour refrigerants Inbrifiants stabilisées Download PDF

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Publication number
EP0773281A2
EP0773281A2 EP96250190A EP96250190A EP0773281A2 EP 0773281 A2 EP0773281 A2 EP 0773281A2 EP 96250190 A EP96250190 A EP 96250190A EP 96250190 A EP96250190 A EP 96250190A EP 0773281 A2 EP0773281 A2 EP 0773281A2
Authority
EP
European Patent Office
Prior art keywords
additive mixture
weight
mixture according
cooling lubricant
stabilizer
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
Application number
EP96250190A
Other languages
German (de)
English (en)
Other versions
EP0773281B1 (fr
EP0773281A3 (fr
Inventor
Wolfgang Siegert
Wolfgang Dr. Beilfuss
Klaus Dr. Weber
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Schuelke and Mayr GmbH
Original Assignee
Schuelke and Mayr GmbH
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Schuelke and Mayr GmbH filed Critical Schuelke and Mayr GmbH
Publication of EP0773281A2 publication Critical patent/EP0773281A2/fr
Publication of EP0773281A3 publication Critical patent/EP0773281A3/fr
Application granted granted Critical
Publication of EP0773281B1 publication Critical patent/EP0773281B1/fr
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

Links

Classifications

    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10MLUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
    • C10M135/00Lubricating compositions characterised by the additive being an organic non-macromolecular compound containing sulfur, selenium or tellurium
    • C10M135/32Heterocyclic sulfur, selenium or tellurium compounds
    • C10M135/36Heterocyclic sulfur, selenium or tellurium compounds the ring containing sulfur and carbon with nitrogen or oxygen
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10MLUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
    • C10M2201/00Inorganic compounds or elements as ingredients in lubricant compositions
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10MLUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
    • C10M2201/00Inorganic compounds or elements as ingredients in lubricant compositions
    • C10M2201/06Metal compounds
    • C10M2201/061Carbides; Hydrides; Nitrides
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10MLUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
    • C10M2201/00Inorganic compounds or elements as ingredients in lubricant compositions
    • C10M2201/16Carbon dioxide
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10MLUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
    • C10M2201/00Inorganic compounds or elements as ingredients in lubricant compositions
    • C10M2201/18Ammonia
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10MLUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
    • C10M2219/00Organic non-macromolecular compounds containing sulfur, selenium or tellurium as ingredients in lubricant compositions
    • C10M2219/10Heterocyclic compounds containing sulfur, selenium or tellurium compounds in the ring
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10MLUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
    • C10M2219/00Organic non-macromolecular compounds containing sulfur, selenium or tellurium as ingredients in lubricant compositions
    • C10M2219/10Heterocyclic compounds containing sulfur, selenium or tellurium compounds in the ring
    • C10M2219/102Heterocyclic compounds containing sulfur, selenium or tellurium compounds in the ring containing sulfur and carbon only in the ring
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10MLUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
    • C10M2219/00Organic non-macromolecular compounds containing sulfur, selenium or tellurium as ingredients in lubricant compositions
    • C10M2219/10Heterocyclic compounds containing sulfur, selenium or tellurium compounds in the ring
    • C10M2219/104Heterocyclic compounds containing sulfur, selenium or tellurium compounds in the ring containing sulfur and carbon with nitrogen or oxygen in the ring
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10MLUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
    • C10M2219/00Organic non-macromolecular compounds containing sulfur, selenium or tellurium as ingredients in lubricant compositions
    • C10M2219/10Heterocyclic compounds containing sulfur, selenium or tellurium compounds in the ring
    • C10M2219/104Heterocyclic compounds containing sulfur, selenium or tellurium compounds in the ring containing sulfur and carbon with nitrogen or oxygen in the ring
    • C10M2219/106Thiadiazoles
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10NINDEXING SCHEME ASSOCIATED WITH SUBCLASS C10M RELATING TO LUBRICATING COMPOSITIONS
    • C10N2040/00Specified use or application for which the lubricating composition is intended
    • C10N2040/20Metal working

Definitions

  • the present invention relates to additive mixtures for cooling lubricant products and cooling lubricant products which contain an isothiazolone and a stabilizer which is effective against chemical decomposition of the isothiazolone.
  • Isothiazolone compounds are known to be effective bactericidal and / or fungicidal active ingredients in cooling lubricants for metalworking.
  • certain components in metalworking fluids tend to destroy the isothiazolones and thus eliminate their microbiological protective activity. This is particularly the case when the metalworking fluids are in a concentrated form.
  • microbicides that are present in combination with isothiazolones can also attack isothiazolones.
  • An example of this is the sodium salt of 2-mercapto-pyridine-N-oxide (sodium omadine) that 5-chloro-2-methyl-isothiazolone decomposes in any system in which both are present together.
  • isothiazolones can be stabilized against chemical decomposition by adding a metal nitrite or a metal nitrate. It is further disclosed that other common salts, including carbonates, sulfates, chlorates, perchlorates and chlorides, are not effective in stabilizing isothiazolone solutions.
  • EP-A-0 425 143, US-A-4 150 026 and US-A-4 241 214 disclose that metal salt complexes of isothiazolones are useful because of their improved thermal stability while maintaining biological activity.
  • EP-B-0 443 821 are additive mixtures for cooling lubricant products which, according to the preamble of claim 1, contain an isothiazolone and a stabilizer which is effective against chemical decomposition of the isothiazolone.
  • an isothiazolone and a stabilizer which is effective against chemical decomposition of the isothiazolone.
  • sulfur-containing compounds or salts thereof which with the Isothiazolone can reversibly form an adduct, especially compounds in which a sulfur atom is attached to an aromatic ring containing nitrogen.
  • Suitable compounds are (in EP-B-0 443 821) 4-mercaptopyridine, the sodium salt of 2-mercaptopyridine, 2-mercaptobenzothiazole and 4-methyl-4-H-1,2,4-triazole-3-thiol .
  • Other compounds mentioned are 2-methylthiobenzothiazole, 2-thiohydantoin, methylene bisthiocyanate, L-cystine and 4-R (thiazolidene-thione-4-carboxylic acid).
  • the ratio of stabilizer to isothiazolone effective for stabilization is at least 0.1: 1, in particular between 0.5: 1 and 1.5: 1.
  • compositions of isothiazolone and stabilizer known from EP-B-0 443 821 can additionally contain solvents.
  • Preferred solvents are so-called "capped polyols", e.g. Triethylene glycol dimethyl ether.
  • the object of the present invention to provide additive mixtures for cooling lubricant products which contain isothiazolones as bactericidal and / or fungicidal active ingredients, which protect cooling lubricant concentrates or cooling lubricants produced therefrom from microbial attack and improve the durability and service life of the cooling lubricant products.
  • the additive mixtures according to the invention should themselves be sufficiently stable and storable and durable under practical conditions.
  • compositions containing isothiazolone and stabilizer in such a way that they can be metered easily into commercially available cooling lubricants, for example by adding a liquid preparation.
  • the metering should be possible in a coolant concentrate or in a coolant, preferably a water-mixed coolant.
  • a solubilizer is additionally provided in the additive mixtures, which is selected from phenoxyethanol, phenoxypropanols, phenoxybutanols, dipropylene glycol, 1-methoxypropanol-2, butyl diglycol and mixtures thereof.
  • the solubilizer is preferably phenoxyethanol, phenoxypropanol or 1-methoxypropanol-2.
  • the solubilizer is, for example, in an amount of 30 to 91.7% by weight, for example 30 to 75, preferably 40 to 70% by weight, more preferably 50 to 65% by weight and in particular approximately 58% by weight Additive mixture included.
  • the cooling lubricant products contain an additive mixture according to the invention.
  • the cooling lubricant products can be present as a cooling lubricant concentrate or contain the cooling lubricant concentrate. Accordingly, the additives according to the invention can be introduced into cooling lubricant concentrates, which are subsequently diluted to cooling lubricants.
  • the cooling lubricant products can be in the form of a solution or an emulsion. Water-mixed cooling lubricants are preferably produced.
  • the isothiazolones used in the additive mixture according to the invention include those which are known from EP-B-0 443 821.
  • Y is a (C 1 -C 18 ) alkyl or (C 3 -C 12 ) cycloalkyl group which is linked to one or more hydroxyl, halogen, cyano, alkylamino, dialkylamino, aryl, amino, Carboxy, carbalkoxy, alkoxy, aryloxy, alkylthio, arylthio, haloalkoxy, cycloalkylamino, carbamoxy or isothiazolonyl groups, an unsubstituted or halogen-substituted (C 2 -C 8 ) alkenyl or - Alkynyl group, a (C 7 -C 10 ) aralkyl group which may be substituted with one or more halogen atoms or one or more (
  • Suitable stabilizers or stabilizer mixtures for the isothiazolone compounds are the compounds known from the prior art, and in particular sulfur-containing compounds or salts thereof, which are reversible with the isothiazolone Can form an adduct.
  • Heterocyclic sulfur-nitrogen compounds such as 2-mercaptopyridine-N-oxide and corresponding salts, preferably alkali metal or ammonium salts such as pyrion-Na (40% aqueous solution of 2-mercaptorpyridine-N-oxide sodium salt) are particularly suitable.
  • 2-mercaptopyridine-N-oxide metal salt complexes such as zinc-pyrithione (e.g.
  • TCMTB Thiocyanatomethyl thio-benzothiazole
  • pyrion-Na, zinc pyrithione, pyrion disulfide and 2-mercaptobenzothiazole are preferred.
  • mild oxidizing agents such as iodopropynyl butyl carbamate, hydrogen peroxide, t-butyl hydroperoxide, sodium bromate and Cu (II) salts are also suitable as stabilizers or co-stabilizers according to the invention, sodium bromate, hydrogen peroxide, 2-tert-butyl-6-methylphenol and pyrion disulfidals Co-stabilizers are preferred.
  • the isothiazolone content in the additive mixture can be 2.25 to 20.25% by weight, for example 6.75 to 20.25% by weight, preferably 9 to 13.5% by weight and in particular approximately 11 % By weight.
  • the stabilizer content in the additive mixture can be approximately 1.3 to 10% by weight, for example 4 to 10% by weight, preferably 6 to 8% by weight and in particular approximately 7% by weight, with for example also 0.05 up to 1.0, preferably 0.5 to 0.1% by weight, in particular 0.2% by weight, of cocatalyst can be present.
  • the molar ratio of isothiazolone compound: stabilizer is, for example, at least 10: 1, preferably between 1.5: 1 and 1: 1.5 and in particular about 1: 1, such as between 1.1: 1 and 1: 1.27.
  • the additive mixtures are preferably incorporated into commercially available coolant concentrates, from which dilutions with water are then made, e.g. 4% dilutions.
  • the liquid preparations can optionally contain further additives which support the functional properties of the cooling lubricant or cooling lubricant additive.
  • the active ingredient isothiazolone
  • the stabilizer for example Pyrion-Na
  • the preparation is easy to dose and can be stored and stored even under practical conditions.
  • the ease of handling of the preparation is also advantageous compared to the storage, preparation and metering of active ingredients and stabilizers present in two-component systems.
  • the additive mixtures according to the invention can be added effectively to cooling lubricant concentrates, so that their durability and the service life of the finished cooling lubricant products are improved compared to known systems.
  • the increased stability of the preparations according to the invention is particularly evident in the lower tendency to form sediments.
  • Kathon RH 893 denotes a 45% n-octylisothiazolone solution in 1,2-propylene glycol and Pyrion-Na a 40% aqueous 2-mercaptopyridine-N-oxide sodium salt solution.
  • Formulations based on Kathon 893 and Pyrion-Na (40%) were dissolved in a molar ratio of 1: 1 to 1: 5 in various solubilizers and examined for compatibility and stability.
  • the total active substance content (sum of N-octylisothiazolone and 2-mercaptopyridine-N-oxide-Na salt) was approx. 18%.
  • a Boko and Lager Boko test (10 days storage of the cooling lubricant concentrate at 40 ° C) was carried out using the samples A, B, C from Example 6 (preparations based on Kathon 893, Pyrion-Na and solubilizers), the individual active ingredients and a combination of the active ingredients NOITZ (Kathon 893 was used) and Na-Pyrion.
  • the preparations or active ingredients were incorporated into the concentrates, from which 4% dilutions were then made in Norderstedter city water.
  • Kathon 893, Pyrion-Na and the solubilizer according to the invention not only facilitated the handling and metering of the agent, it also improved the stability and the effectiveness of the biocide mixture.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Organic Chemistry (AREA)
  • Agricultural Chemicals And Associated Chemicals (AREA)
  • Thiazole And Isothizaole Compounds (AREA)
  • Lubricants (AREA)
EP96250190A 1995-09-08 1996-09-05 Préparations pour refrigerants Inbrifiants stabilisées Expired - Lifetime EP0773281B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE19534532A DE19534532C2 (de) 1995-09-08 1995-09-08 Additivmischungen für Kühlschmiermittelprodukte und deren Verwendung
DE19534532 1995-09-08

Publications (3)

Publication Number Publication Date
EP0773281A2 true EP0773281A2 (fr) 1997-05-14
EP0773281A3 EP0773281A3 (fr) 1998-05-13
EP0773281B1 EP0773281B1 (fr) 2005-10-19

Family

ID=7772453

Family Applications (1)

Application Number Title Priority Date Filing Date
EP96250190A Expired - Lifetime EP0773281B1 (fr) 1995-09-08 1996-09-05 Préparations pour refrigerants Inbrifiants stabilisées

Country Status (3)

Country Link
EP (1) EP0773281B1 (fr)
DE (2) DE19534532C2 (fr)
ES (1) ES2247597T3 (fr)

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6211213B1 (en) * 1999-04-16 2001-04-03 Rohm And Haas Company Stable microbicide formulation
WO2002067685A1 (fr) * 2001-02-26 2002-09-06 Lonza Inc. Preparations de conservateurs stables comprenant des composes halopropynyle et un solvant butoxydiglycol
US6607738B2 (en) 1997-04-24 2003-08-19 Nipa Laboratories, Ltd. Chemical composition
EP1332675A3 (fr) * 2002-01-31 2003-10-01 Rohm and Haas Associations microbicides synergiques
EP1514473A1 (fr) * 2003-09-04 2005-03-16 Air Liquide Santé (International) Composition microbicide à faible teneur en sels ou exempte de ceux-ci à base de dérivés d'isothiazolone et de pyrion disulfure
US9034905B2 (en) 2003-02-05 2015-05-19 Rohm And Haas Company Synergistic microbicidal combinations

Families Citing this family (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB2320026B (en) 1996-12-05 2000-01-26 Sunkyong Ind Ltd Stabilized isothiazolone solution
DE19961621C2 (de) * 1999-12-13 2002-11-14 Schuelke & Mayr Gmbh Bakterizide und fungizide flüssige Zubereitungen für technische Produkte
DE102004052878A1 (de) 2004-11-02 2006-05-04 Schülke & Mayr GmbH Isothiazolonhaltige Konservierungsmittel mit verbesserter Stabilität
DE102006045066B4 (de) * 2006-09-21 2010-07-01 Schülke & Mayr GmbH Mikrobizide Zubereitung auf der Basis von 1,2-Benzisothiazolin-3-on mit einem Gehalt an aromatischem Alkohol
DE102009048189A1 (de) * 2009-10-02 2011-04-07 Schülke & Mayr GmbH Lagerstabile mikrobizide Konzentrate und deren Verwendung als Konservierungsmittel

Family Cites Families (12)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3870795A (en) * 1973-02-28 1975-03-11 Rohm & Haas Stabilization of solutions of 3-isothiazolones employing certain metal nitrates and nitrites
DE3904099C1 (fr) * 1989-02-11 1990-07-12 Schuelke & Mayr Gmbh, 2000 Norderstedt, De
DE3911808A1 (de) * 1989-04-11 1990-10-18 Riedel De Haen Ag Fluessiges konservierungsmittel
DE58906847D1 (de) * 1989-11-10 1994-03-10 Thor Chemie Gmbh Stabilisierte wässrige Lösungen von 3-Isothiazolinonen.
GB9003871D0 (en) * 1990-02-21 1990-04-18 Rohm & Haas Stabilization of isothiazolones
US5037989A (en) * 1990-04-05 1991-08-06 Rohm And Haas Company Phenoxyalkanol as a stabilizer for isothiazolone concentrates
US5108500A (en) * 1990-12-10 1992-04-28 Rohm And Haas Company Stabilization of water insoluble 3-isothiazolones
JP3524937B2 (ja) * 1992-02-10 2004-05-10 日本エンバイロケミカルズ株式会社 工業用殺菌剤
GB9300936D0 (en) * 1993-01-19 1993-03-10 Zeneca Ltd Stable liquid compositions and their use
JPH07133205A (ja) * 1993-11-08 1995-05-23 Shinto Paint Co Ltd 木材用防カビ組成物
US5478797A (en) * 1994-11-21 1995-12-26 Rohm And Haas Company Bromate stabilization of nitrate-free 3-isothiazolones at pH 4-5.1
US5599827A (en) * 1995-05-16 1997-02-04 Rohm And Haas Company Stable microemulsions of certain 3-isothiazolone compounds

Cited By (16)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6607738B2 (en) 1997-04-24 2003-08-19 Nipa Laboratories, Ltd. Chemical composition
US6211213B1 (en) * 1999-04-16 2001-04-03 Rohm And Haas Company Stable microbicide formulation
WO2002067685A1 (fr) * 2001-02-26 2002-09-06 Lonza Inc. Preparations de conservateurs stables comprenant des composes halopropynyle et un solvant butoxydiglycol
EP1332675A3 (fr) * 2002-01-31 2003-10-01 Rohm and Haas Associations microbicides synergiques
EP1488699A1 (fr) * 2002-01-31 2004-12-22 Rohm And Haas Company Associations microbicides synergiques
US9426994B2 (en) 2003-02-05 2016-08-30 Rohm And Haas Company Synergistic microbicidal combinations
US9034905B2 (en) 2003-02-05 2015-05-19 Rohm And Haas Company Synergistic microbicidal combinations
US9426993B2 (en) 2003-02-05 2016-08-30 Rohm And Haas Company Synergistic microbicidal combinations
US9474280B2 (en) 2003-02-05 2016-10-25 Rohm And Haas Company Synergistic microbicidal combinations
US9480258B2 (en) 2003-02-05 2016-11-01 Rohm And Haas Company Synergistic microbicidal combinations
US9491945B2 (en) 2003-02-05 2016-11-15 Rohm And Haas Company Synergistic microbicidal combinations
US9497968B2 (en) 2003-02-05 2016-11-22 Rohm And Haas Company Synergistic microbicidal combinations
US9497969B2 (en) 2003-02-05 2016-11-22 Rohm And Haas Company Synergistic microbicidal combinations
US9532571B2 (en) 2003-02-05 2017-01-03 Rohm And Haas Company Synergistic microbicidal combinations
JP2005082596A (ja) * 2003-09-04 2005-03-31 L'air Liquide Sante Internatl イソチアゾロン誘導体およびピリオンジスルフィドに基づく低塩含量または塩フリーの殺菌剤組成物
EP1514473A1 (fr) * 2003-09-04 2005-03-16 Air Liquide Santé (International) Composition microbicide à faible teneur en sels ou exempte de ceux-ci à base de dérivés d'isothiazolone et de pyrion disulfure

Also Published As

Publication number Publication date
DE19534532C2 (de) 1999-04-08
EP0773281B1 (fr) 2005-10-19
DE19534532A1 (de) 1997-03-20
ES2247597T3 (es) 2006-03-01
EP0773281A3 (fr) 1998-05-13
DE59611282D1 (de) 2006-03-02

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