EP1077250B1 - Wässrige Reinigungsformulierungen - Google Patents
Wässrige Reinigungsformulierungen Download PDFInfo
- Publication number
- EP1077250B1 EP1077250B1 EP00305606A EP00305606A EP1077250B1 EP 1077250 B1 EP1077250 B1 EP 1077250B1 EP 00305606 A EP00305606 A EP 00305606A EP 00305606 A EP00305606 A EP 00305606A EP 1077250 B1 EP1077250 B1 EP 1077250B1
- Authority
- EP
- European Patent Office
- Prior art keywords
- composition
- weight
- quaternary ammonium
- sodium
- surfactant
- 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.)
- Expired - Lifetime
Links
Classifications
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/02—Inorganic compounds ; Elemental compounds
- C11D3/04—Water-soluble compounds
- C11D3/044—Hydroxides or bases
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D1/00—Detergent compositions based essentially on surface-active compounds; Use of these compounds as a detergent
- C11D1/66—Non-ionic compounds
- C11D1/825—Mixtures of compounds all of which are non-ionic
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D1/00—Detergent compositions based essentially on surface-active compounds; Use of these compounds as a detergent
- C11D1/88—Ampholytes; Electroneutral compounds
- C11D1/94—Mixtures with anionic, cationic or non-ionic compounds
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/02—Inorganic compounds ; Elemental compounds
- C11D3/04—Water-soluble compounds
- C11D3/08—Silicates
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/48—Medical, disinfecting agents, disinfecting, antibacterial, germicidal or antimicrobial compositions
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D1/00—Detergent compositions based essentially on surface-active compounds; Use of these compounds as a detergent
- C11D1/38—Cationic compounds
- C11D1/62—Quaternary ammonium compounds
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D1/00—Detergent compositions based essentially on surface-active compounds; Use of these compounds as a detergent
- C11D1/66—Non-ionic compounds
- C11D1/662—Carbohydrates or derivatives
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D1/00—Detergent compositions based essentially on surface-active compounds; Use of these compounds as a detergent
- C11D1/88—Ampholytes; Electroneutral compounds
- C11D1/883—Aminimide, i.e. ammonioamidates
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D1/00—Detergent compositions based essentially on surface-active compounds; Use of these compounds as a detergent
- C11D1/88—Ampholytes; Electroneutral compounds
- C11D1/90—Betaines
Definitions
- This invention relates to cleaning formulations and in particular to formulations for use in the cleaning of milking and milk storage equipment such as bulk milk tanks, milk pipelines.
- cleaning formulations for milking and milk storage equipment have been based on combinations of alkaline compounds (sodium hydroxide, potassium hydroxide, sodium carbonate) in solution with sodium hypochlorite for sanitising.
- alkaline compounds sodium hydroxide, potassium hydroxide, sodium carbonate
- sodium hypochlorite is a very effective sanitising agent
- its solutions do not wet surfaces very effectively and hence products have been developed to overcome this wetting problem.
- Surfactants have been found to increase wetting power and hence may be added to sodium hypochlorite formulations.
- only a limited number of surfactants are compatible with sodium hypochlorite and these surfactants are usually high foaming.
- Such high foaming formulations do not work well in certain environments such as cleaning in place (CIP) in milk and food pipeline systems.
- Sodium hypochlorite solutions containing sodium hydroxide are alkaline and corrosive and hence are not suitable for use with milking equipment or milk storage systems comprising metals such as aluminium or zinc or soft metal alloys.
- the reaction between the formulation and metal may also produce hydrogen which may have a corrosive effect on equipment structures.
- a range of alternative products have been developed which have disinfectant properties, for example products comprising quaternary ammonium compounds (cationics), amphoterics, iodine compounds. None of these products are as efficient as formulations comprising sodium hypochlorite and most cannot be used in alkaline mixtures. Since a level of causticity is required to emulsify fats and ensure successful removal of protein deposits from milking equipment, such as bulk storage tanks, such alternative products are also not favoured.
- an alkaline formulation including surfactants, disinfectants, a hydrotroping agent and optionally a scale build-up retardant can provide efficacious sanitising with low foaming properties which is a real alternative to alkaline formulations containing sodium hypochlorite.
- the invention thus provides an aqueous cleaning composition according to claim 1.
- Preferred metal hydroxides are potassium hydroxide and especially sodium hydroxide.
- Preferred metal silicates are sodium silicate, especially sodium metasilicate.
- the alkalinity is provided by sodium hydroxide alone.
- the formulation contains 2 to 25%, preferably 5 to 15%, more preferably 6 to 10% by weight of the metal hydroxide and/or metal silicate component. Surprisingly it has been found that the surfactants, disinfectant and hydrotroping agent can tolerate these high levels of causticity.
- the surfactant mixture comprises both an alkyl glucoside and a specific nonionic surfactant.
- Alkyl glucosides also known as sugar lipids, are commercially available from a variety of suppliers and have a range of applications and properties. Alkyl glucosides are derived from glucose and possess alkyl substituents of differing chain length, for example C 3-14
- alkoxylate surfactants of general formula R(O(CH 2 ) m ) n OH where R is an alkyl group with an active hydrogen atom, e.g. an amine, alcohol, fatty acid, ester; m is 2 or 3, preferably 2; and n is 4 to 20 are commercially available.
- R is an alkyl group with an active hydrogen atom, e.g. an amine, alcohol, fatty acid, ester; m is 2 or 3, preferably 2; and n is 4 to 20 are commercially available.
- a particularly useful combination of alkyl glucoside and ethoxylate surfactant is sold under the trade name Berol by Akzo-Nobel, specifically Berol LFG 61 or Berol DGR 81.
- the formulation of the invention contains 2 to 15%, preferably 5 to 9%, especially 5 to 7% by weight of the surfactant component.
- Other suitable surfactant mixtures will of course be readily determined by the person skilled in the art.
- Quaternary ammonium disinfectants are also commercially available. They are typically of formula RN(CH 3 ) 3 Cl where R is C 6-20 alkyl. One of the methyl groups is often replaced by a longer alkyl chain, e.g. a C 2-20 or C 6-20 alkyl chain, giving alternative quaternary ammonium disinfectants.
- a particularly useful quaternary ammonium disinfectant is dioctyldimethylammonium chloride which is sold under the trade name Bardac-LF by Lonza.
- the formulation of the invention contains 0.5 to 10%, preferably 1 to 7%, especially 2 to 5% by weight of the quaternary ammonium disinfectant.
- Other suitable quaternary ammonium disinfectants will of course be readily determined by the person skilled in the art.
- the hydrotroping agent is a propionate, betaine or glycinate type of amphoteric surfactant and a range of such hydrotroping agents are again readily available in the market place.
- Particularly preferred hydrotroping agents include octylimino-dipropionate and sodium capryloimino-dipropionate.
- a particularly useful hydrotroping agent is that sold under the trade name Ampholak YJH-40 by Akzo-Nobel.
- the formulation contains 1 to 10%, preferably 2 to 8%, especially 3 to 7% by weight of the hydrotroping agent.
- a chelating agent in the formulations of the invention, especially in areas of hard water.
- a chelating agent this may conveniently be trisodium nitrilotriacetate (sodium NTA) or 2-phosphonobutane-1,2,4-tricarboxylic acid (PBTC) or its sodium salts.
- the formulation of the invention contains 1 to 10%, preferably 2 to 8%, especially 3 to 5% by weight of the chelating agent.
- Other suitable chelating agents will of course be readily determined by the person skilled in the art.
- the balance of the cleaning formulation of the invention is water.
- the formulation is further diluted with water at a ratio of 200-300:1 water/cleaner.
- sanitisation occurs at elevated temperature, e.g. 30°C, especially 75°C. This has been found to enhance the effectiveness of the sanitising formulation to bacteria.
- a tap water sample was inoculated with high numbers (10 6 ) of Bacillus cereus .
- Another tap water sample was injected with high numbers of E.Coli .
- Both samples were divided into four separate tubes and a formulation comprising 7.5% by weight sodium hydroxide, 6.0% by weight Berol LFG61, 3.0% by weight Bardac LF, 4.5% by weight Ampholak YJH-40, 4% sodium NTA and 75% by weight water was added to a tube from each set to give a final dilution of 1:300, 1:250 and 1:200 respectively.
- the remaining two tubes were kept as controls. All the tubes were incubated at 30°C for 10 minutes. The results are displayed in Table 1 below.
Claims (12)
- Wässrige Reinigungszusammensetzung, umfassend:(i) 2 bis 25 Gewichts-% von mindestens einem Metallhydroxid und/oder Metallsilikat;(ii) eine Tensidmischung umfassend mindestens ein Alkylglukosid und mindestens ein Alkoxylat-Tensid der allgemeinen Formel R(O(CH2)m)nOH, wobei R eine Alkylgruppe mit einem aktiven Wasserstoffatom ist; m 2 oder 3 ist; und n 4 bis 20 ist;(iii) ein quartäres Ammonium-Desinfektionsmittel;(iv) ein hydrotropes Mittel, das ein amphoteres Propionat-, Betain- oder Glycinat-Tensid ist; und(v) optional ein chelatbildendes Mittel.
- Zusammensetzung nach Anspruch 1, wobei das Metallhydroxid und/oder Metallsilikat Kaliumhydroxid, Natriumhydroxid und/oder Natriumsilikat ist.
- Zusammensetzung nach einem der vorhergehenden Ansprüche, umfassend 2 bis 15 Gewichts-% Tensidmischung.
- Zusammensetzung nach einem der vorhergehenden Ansprüche, wobei das quartäre Ammonium-Desinfektionsmittel die Formel RN(CH3)3Cl aufweist, wobei R C6-20-Alkyl ist.
- Zusammensetzung nach Anspruch 4, wobei eine der Methylgruppen in der Formel RN(CH3)3Cl durch ein C6-20-Alkyl ersetzt ist.
- Zusammensetzung nach Anspruch 4, wobei das quartäre Ammonium-Desinfektionsmittel Dioctyldimethylammoniumchlorid ist.
- Zusammensetzung nach einem der vorhergehenden Ansprüche, umfassend 0,5 bis 10 Gewichts-% quartäres Ammonium-Desinfektionsmittel.
- Zusammensetzung nach einem der vorhergehenden Ansprüche, wobei das hydrotrope Mittel Octyliminodipropionat oder Natriumcapryliminodipropionat ist.
- Zusammensetzung nach einem der vorhergehenden Ansprüche, umfassend 1 bis 10 Gewichts-% hydrotropes Mittel.
- Zusammensetzung nach einem der vorhergehenden Ansprüche, umfassend ein chelatbildendes Mittel, das Trinatriumnitrilotriacetat (Natrium-NTA) oder 2-Phosphonobutan-1,2,4-Tricarbonsäure (PBTC) oder ein Natriumsalz davon ist.
- Verwendung einer Zusammensetzung nach einem der Ansprüche 1 bis 10 bei der Reinigung von Melk- und Milchlagerungs-Einrichtungen.
- Zusammensetzung nach Anspruch 1, bestehend aus:(i) 2 bis 25 Gewichts-% von mindestens einem Metallhydroxid und/oder Metallsilikat;(ii) einer Tensidmischung, im wesentlichen bestehend aus mindestens einem Alkylglukosid und mindestens einem Alkoxylat-Tensid der allgemeinen Formel R(O(CH2)m)nOH, wobei R eine Alkylgruppe mit einem aktiven Wasserstoffatom ist; m 2 oder 3 ist; und n 4 bis 20 ist;(iii) einem quartären Ammonium-Desinfektionsmittel;(iv) einem hydrotropen Mittel, das ein amphoteres Propionat-, Betain- oder Glycinat-Tensid ist;(v) optional einem chelatbildenden Mittel; und(vi) Wasser.
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
GBGB9919324.5A GB9919324D0 (en) | 1999-08-16 | 1999-08-16 | Formulations |
GB9919324 | 1999-08-16 |
Publications (2)
Publication Number | Publication Date |
---|---|
EP1077250A1 EP1077250A1 (de) | 2001-02-21 |
EP1077250B1 true EP1077250B1 (de) | 2005-01-26 |
Family
ID=10859219
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP00305606A Expired - Lifetime EP1077250B1 (de) | 1999-08-16 | 2000-07-03 | Wässrige Reinigungsformulierungen |
Country Status (5)
Country | Link |
---|---|
EP (1) | EP1077250B1 (de) |
AT (1) | ATE287941T1 (de) |
DE (1) | DE60017648T2 (de) |
DK (1) | DK1077250T3 (de) |
GB (1) | GB9919324D0 (de) |
Cited By (10)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US8262805B2 (en) | 2010-08-23 | 2012-09-11 | Ecolab Usa Inc. | Poly sulfonate functionalized alkyl polyglucosides for enhanced food soil removal |
US8283302B2 (en) | 2010-06-21 | 2012-10-09 | Ecolab Usa Inc. | Alkyl polypentosides and alkyl polyglucosides (C8-C11) used for enhanced food soil removal |
US8287659B2 (en) | 2010-08-23 | 2012-10-16 | Ecolab Usa Inc. | Poly phosphate functionalized alkyl polyglucosides for enhanced food soil removal |
US8299009B2 (en) | 2010-06-21 | 2012-10-30 | Ecolab Usa Inc. | Betaine functionalized alkyl polyglucosides for enhanced food soil removal |
US8329633B2 (en) | 2010-09-22 | 2012-12-11 | Ecolab Usa Inc. | Poly quaternary functionalized alkyl polyglucosides for enhanced food soil removal |
US8389457B2 (en) | 2010-09-22 | 2013-03-05 | Ecolab Usa Inc. | Quaternary functionalized alkyl polyglucosides for enhanced food soil removal |
US8658584B2 (en) | 2010-06-21 | 2014-02-25 | Ecolab Usa Inc. | Sulfosuccinate functionalized alkyl polyglucosides for enhanced food and oily soil removal |
US8877703B2 (en) | 2010-09-22 | 2014-11-04 | Ecolab Usa Inc. | Stearyl and lauryl dimoniumhydroxy alkyl polyglucosides for enhanced food soil removal |
WO2023275269A1 (en) * | 2021-06-30 | 2023-01-05 | Nouryon Chemicals International B.V. | Chelate-amphoteric surfactant liquid concentrates and use thereof in cleaning applications |
US11834624B2 (en) | 2014-03-07 | 2023-12-05 | Ecolab Usa Inc. | Alkyl amides for enhanced food soil removal and asphalt dissolution |
Families Citing this family (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE10144187B4 (de) * | 2001-09-07 | 2007-12-13 | Schülke & Mayr GmbH | Konservierungsmittel für Beschichtungszusammensetzungen |
US8232239B2 (en) | 2010-03-09 | 2012-07-31 | Ecolab Usa Inc. | Liquid concentrated fabric softener composition |
US8460477B2 (en) | 2010-08-23 | 2013-06-11 | Ecolab Usa Inc. | Ethoxylated alcohol and monoethoxylated quaternary amines for enhanced food soil removal |
US9089251B2 (en) | 2011-10-14 | 2015-07-28 | Ecolab Usa Inc. | Method of removing and preventing redeposition of protein soils using sugar esters |
Citations (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US5102874A (en) * | 1986-08-25 | 1992-04-07 | Ecolab Inc. | Antimicrobial mixtures containing quaternary ammonium compounds and a quaternary phosphonium compounds |
WO1999019438A1 (en) * | 1997-10-15 | 1999-04-22 | Stepan Company | High foaming detergent composition having non-ionic surfactant base |
Family Cites Families (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
SU735630A1 (ru) * | 1975-03-20 | 1980-05-25 | Ереванский Зоотехнический Ветеринарный Институт | Моющее средство дл обработки молочного оборудовани |
US4240921A (en) * | 1979-03-28 | 1980-12-23 | Stauffer Chemical Company | Liquid cleaning concentrate |
RU2010844C1 (ru) * | 1992-02-04 | 1994-04-15 | Московский институт прикладной биотехнологии | Моющее средство для очистки коптильных камер и труб дымоходов |
JP4114820B2 (ja) * | 1995-12-11 | 2008-07-09 | 昭和電工株式会社 | 洗浄剤組成物 |
RU2129591C1 (ru) * | 1997-06-11 | 1999-04-27 | Товарищество с ограниченной ответственностью "Экохиммаш" | Моющее средство для обработки молочного оборудования |
-
1999
- 1999-08-16 GB GBGB9919324.5A patent/GB9919324D0/en not_active Ceased
-
2000
- 2000-07-03 AT AT00305606T patent/ATE287941T1/de not_active IP Right Cessation
- 2000-07-03 EP EP00305606A patent/EP1077250B1/de not_active Expired - Lifetime
- 2000-07-03 DE DE60017648T patent/DE60017648T2/de not_active Expired - Fee Related
- 2000-07-03 DK DK00305606T patent/DK1077250T3/da active
Patent Citations (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US5102874A (en) * | 1986-08-25 | 1992-04-07 | Ecolab Inc. | Antimicrobial mixtures containing quaternary ammonium compounds and a quaternary phosphonium compounds |
WO1999019438A1 (en) * | 1997-10-15 | 1999-04-22 | Stepan Company | High foaming detergent composition having non-ionic surfactant base |
Cited By (13)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US8283302B2 (en) | 2010-06-21 | 2012-10-09 | Ecolab Usa Inc. | Alkyl polypentosides and alkyl polyglucosides (C8-C11) used for enhanced food soil removal |
US8299009B2 (en) | 2010-06-21 | 2012-10-30 | Ecolab Usa Inc. | Betaine functionalized alkyl polyglucosides for enhanced food soil removal |
US8658584B2 (en) | 2010-06-21 | 2014-02-25 | Ecolab Usa Inc. | Sulfosuccinate functionalized alkyl polyglucosides for enhanced food and oily soil removal |
US8262805B2 (en) | 2010-08-23 | 2012-09-11 | Ecolab Usa Inc. | Poly sulfonate functionalized alkyl polyglucosides for enhanced food soil removal |
US8287659B2 (en) | 2010-08-23 | 2012-10-16 | Ecolab Usa Inc. | Poly phosphate functionalized alkyl polyglucosides for enhanced food soil removal |
US8557760B2 (en) | 2010-09-22 | 2013-10-15 | Ecolab Usa Inc. | Quaternary functionalized alkyl polyglucosides for enhanced food soil removal |
US8389457B2 (en) | 2010-09-22 | 2013-03-05 | Ecolab Usa Inc. | Quaternary functionalized alkyl polyglucosides for enhanced food soil removal |
US8329633B2 (en) | 2010-09-22 | 2012-12-11 | Ecolab Usa Inc. | Poly quaternary functionalized alkyl polyglucosides for enhanced food soil removal |
US8877703B2 (en) | 2010-09-22 | 2014-11-04 | Ecolab Usa Inc. | Stearyl and lauryl dimoniumhydroxy alkyl polyglucosides for enhanced food soil removal |
US10035975B2 (en) | 2010-09-22 | 2018-07-31 | Ecolab Usa Inc. | Stearyl and lauryl dimoniumhydroxy alkyl polyglucosides for enhanced food soil removal |
US10655085B2 (en) | 2010-09-22 | 2020-05-19 | Ecolab Usa Inc. | Stearyl and lauryl dimoniumhydroxy alkyl polyglucosides for enhanced food soil removal |
US11834624B2 (en) | 2014-03-07 | 2023-12-05 | Ecolab Usa Inc. | Alkyl amides for enhanced food soil removal and asphalt dissolution |
WO2023275269A1 (en) * | 2021-06-30 | 2023-01-05 | Nouryon Chemicals International B.V. | Chelate-amphoteric surfactant liquid concentrates and use thereof in cleaning applications |
Also Published As
Publication number | Publication date |
---|---|
DK1077250T3 (da) | 2005-05-30 |
DE60017648D1 (de) | 2005-03-03 |
ATE287941T1 (de) | 2005-02-15 |
GB9919324D0 (en) | 1999-10-20 |
EP1077250A1 (de) | 2001-02-21 |
DE60017648T2 (de) | 2006-03-30 |
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