EP0826770A2 - Flüssige Bleichmittelsuspension - Google Patents
Flüssige Bleichmittelsuspension Download PDFInfo
- Publication number
- EP0826770A2 EP0826770A2 EP97114695A EP97114695A EP0826770A2 EP 0826770 A2 EP0826770 A2 EP 0826770A2 EP 97114695 A EP97114695 A EP 97114695A EP 97114695 A EP97114695 A EP 97114695A EP 0826770 A2 EP0826770 A2 EP 0826770A2
- Authority
- EP
- European Patent Office
- Prior art keywords
- anhydride
- liquid bleach
- acid
- liquid
- hydrogen peroxide
- 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.)
- Withdrawn
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
- C11D3/39—Organic or inorganic per-compounds
- C11D3/3947—Liquid 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
- C11D1/66—Non-ionic compounds
- C11D1/825—Mixtures of compounds all of which are non-ionic
- C11D1/8255—Mixtures of compounds all of which are non-ionic containing a combination of compounds differently alcoxylised or with differently alkylated chains
-
- 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
- C11D3/16—Organic compounds
- C11D3/20—Organic compounds containing oxygen
- C11D3/2075—Carboxylic acids-salts thereof
- C11D3/2082—Polycarboxylic acids-salts thereof
-
- 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
- C11D1/72—Ethers of polyoxyalkylene glycols
Definitions
- bleaching power of persalts such as sodium perborates or Percarbonates can be significantly increased by adding a bleach activator can.
- bleach activators are mostly reactive organic compounds with a O-acyl or N-acyl group in alkaline solution together with a source form the corresponding peroxycarboxylic acids for hydrogen peroxide. This already have a good bleaching effect at temperatures below 60 ° C.
- bleach activators are tetraacetylethylenediamine (TAED), Benzoyloxybenzenesulfonate (BOBS), nonanoyloxybenzenesulfonate (NOBS) and Tetraacetylglucoluril (TAGU).
- Further activators are in GB-A-836 988, GB-A-907 356, EP-A-98 129 and EP-A-120 591. Nitriles and Anhydrides, both in cyclic and in open form, are potential Bleach activators.
- aqueous suspensions of organic peracids are available liquid bleach described.
- a suspension of a solid peroxycarboxylic acid in a liquid carrier material described the one contains non-starchy polymer-based thickeners.
- Bleach suspensions based on colloidal silica, xanthan or agar polysaccharides are described in EP-A-283 791 and 283 792.
- EP-A-334 405 and 337 516 organic peracids such as Dodecyldipercarboxylic acid in combination with alkanesulfonate as an anionic surfactant prefers.
- organic peracids such as Dodecyldipercarboxylic acid in combination with alkanesulfonate as an anionic surfactant prefers.
- ethoxylated alcohols EP-A-334 405
- fatty acids EP-A-337 516) possible.
- Suspensions of organic Peroxy carboxylic acids (DPDDA or phthalimidoperoxy carboxylic acid) in nonionic Surfactants with HLB values between 6.5 and 11 are described in EP-A-386 566 and EP-A-497 337.
- alkyl substituted succinic acids in liquid Detergent formulations are known in principle (EP-A-212 723, EP-A-241 073 and WO 92 05 238). These liquid detergents do not contain hydrogen peroxide and the alkyl-substituted succinic acids only serve as builders there. So far, no storage-stable aqueous systems are known that contain an anhydride Contain hydrogen peroxide. Experience has shown that the anhydride should be very good hydrolyze quickly and therefore no activating effect on hydrogen peroxide exercise.
- the surfactant preferably contains the lower content of Ethylene oxide 2-4 units of ethylene oxide and the more highly ethoxylated surfactant preferably 6-12 units of ethylene oxide.
- the basis of these surfactants Alcohols can and can be of natural or petrochemical origin be branched or straight chain. Examples of lower oxyethylated alcohols are ®Genapol UD-030, 050, Genapol C-050, Genapol O-020, 050, Genapol OA-040, Genapol OX-030, Genapol T-050 or Genapol X-030, 050.
- Example for medium or highly ethoxylated alcohols are Genapol OA-070, 080, 089, Genapol OX-060, 080, 100, 109, 130, Genapol O-080, 100, 120, 150, Genapol C-080, 100, Genapol UD-079, 080, 088, 110, Genapol T-080, 100, 110, 150, 180 or Genapol X-060, 080, 150.
- the fatty alcohol residues can be the same or different.
- the mixing ratio of both surfactants can be varied within a wide range.
- Mixing ratios of low to medium or highly ethoxylated are preferred Fatty alcohols from 1: 4 to 4: 1 are particularly preferred Surfactant mixtures in which the surfactants are present in a ratio of 1: 2 to 2: 1.
- an emulsifier is preferred should be stable to oxidation, for example mono-, di- or trialkyl phosphates or their unsaturated variants.
- An example of this is stearyl mono / diphosphate.
- the total content of surfactants in the bleach suspension is 1 to 50, preferably 2 to 30, in particular 3 to 25% by weight.
- cyclic anhydrides which are almost water-insoluble at pH 2-6 and room temperature can be used as bleach activator in the formulations according to the invention.
- Cyclic 5-ring anhydrides which are derived from maleic acid or succinic acid are particularly preferred.
- Particularly preferred compounds are branched or straight-chain, optionally additionally substituted alkyl or alkenyl-substituted maleic or succinic anhydrides of the general formulas wherein RC 1 -C 22 alkyl, C 2 -C 22 alkenyl or phenyl.
- the concentration of the bleach activator in the formulation according to the invention is 0.5-30, preferably 3-20% by weight.
- the liquid bleaching agent suspensions according to the invention contain as an essential component hydrogen peroxide in concentrations between 1 and 30%, preferably 2-10%, calculated as 100% H 2 O 2 . It can be used in commercial form as a 10, 30, 35, 50 or 70% solution.
- the formulations according to the invention can contain stabilizers or complexing agents in order to complex heavy metal ions. Examples of such complexing agents are ethylenediaminetetraacetic acid (EDTA), nitrilotriacetic acid (NTA), isoserinediacetic acid, ethylenediaminetetramethylenephosphonic acid (EDTMP), but especially diethylenetriaminepentamethylenephosphonic acid or substituted triazacyclononanes such as trimethyltriazacyclononane.
- EDTA ethylenediaminetetraacetic acid
- NTA nitrilotriacetic acid
- ETMP ethylenediaminetetramethylenephosphonic acid
- the concentration of these compounds can be between 5 ppm and 8%, preferably 10 ppm - 5%. In special applications e.g. B. for the removal of blood stains, a high concentration (approx. 3 - 5%) of these substances may be desirable.
- the compounds of this type can be added in the form of the free acid, partially neutralized or added as salts.
- the bleaching agent suspensions according to the invention also contain Water in amounts up to 80% by weight.
- pH adjusting agents may also be necessary be, since the formulations optimal chemical stability in acid pH range, in particular between pH 2-8, preferably at pH 3-6. All organic or inorganic acids are used to acidify the suspension such as hydrochloric acid, phosphoric acid, sulfuric acid, acetic acid, citric acid, Lactic acid, for alkalizing inorganic bases or organic amines usable.
- the formulation according to the invention can contain, as further additives, defoamers, optical brighteners, perfumes, dyes, antioxidants or hydrogen peroxide contain.
- the liquid bleaches according to the invention can be found in numerous Use application areas, such. B. as a detergent additive for Textile laundry, as a washing power amplifier, as a light duty liquid, as a cleaning and Disinfectant for hard surfaces, as an all-purpose cleaner or acid Abresive cleaner.
- the bleach can also be used as a soak or stain remover will.
- the highly viscous formulations are particularly suitable for this can be applied directly to soiling.
- Pasty formulations can e.g. B. in tubes or in the form of sticks in the trade.
- the bleach suspension is used in such concentrations that the Active oxygen content of the wash liquor at the start of the washing process 0.5 - 50 ppm, is preferably 3 to 30 ppm active oxygen.
- the emulsifier (stearyl mono / diphosphate) was melted and the bleach activator (i-nonenoylsuccinic anhydride) was added.
- the nonionic surfactants were melted and the mixture, water and complexing agent (®Dequest 2066) described above was added to this melt.
- the formulation was allowed to cool with stirring, the pH was adjusted to 4 with sulfuric acid and then the H 2 O 2 was slowly stirred in and the mixture was homogenized.
- the bleaching effect of the bleaching agent suspensions according to the invention was checked in washing tests.
- the washing tests were carried out in a washing machine (Miele W 723) at 40 ° C. using water with a water hardness of 15 ° dH.
- the bleaching formulation was spread on the test fabric and, after 15 minutes of exposure, was washed in the washing machine with 180 g ®Dash (Procter & Gamble, Italy).
- the main wash time was 70 minutes.
- a formulation according to Example 1 was used in which nonenoylsuccinic anhydride was replaced by acetyl triethyl citrate (ATEC).
- acetyl triethyl citrate AEC
- the washing results demonstrate the bleaching effectiveness of the inventive Wording. After a storage period of 3 months, only an insignificant one Decrease in bleaching activity observed.
Landscapes
- Chemical & Material Sciences (AREA)
- Life Sciences & Earth Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Wood Science & Technology (AREA)
- Organic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Emergency Medicine (AREA)
- Inorganic Chemistry (AREA)
- Detergent Compositions (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
Abstract
Description
Voraussetzung für einen kommerziellen Einsatz solcher flüssiger Bleichmittel auf Basis von Wasserstoffperoxid ist, daß diese Bleichmittel physikalisch stabil sind und sich daher ohne nennenswerten Verlust an Aktivsauerstoff längere Zeit problemlos lagern lassen.
Beispiel | 1 | 2 | 3 | 4 |
C11-Oxoalkohol + 3 EO | 10 | 10 | 5 | 10 |
C14/C15-Oxoalkohol + 8 EO | 10 | 10 | 5 | 5 |
Komplexbildner | 2 | 2 | 1 | 1 |
Bleichaktivator | 5 | 5 | 3 | 6 |
Emulgator | 3 | 1 | 1 | 3 |
H2O2 (35 %ig) | 15 | 15 | 10 | 15 |
dest. Wasser | ad 100 | |||
alle Zahlen bedeuten Gew.-%; EO = Ethylenoxid |
Die Waschversuche wurden in einer Waschmachine (Miele W 723) bei 40 °C unter Verwendung von Wasser der Wasserhärte 15 ° dH durchgeführt. Die Bleichformulierung wurde auf das Testgewebe gestrichen und nach 15 Minuten Einwirkzeit mit 180 g ®Dash (Procter & Gamble, Italien) in der Waschmaschine gewaschen. Die Hauptwaschzeit betrug 70 Minuten. Als Vergleich wurde eine Formulierung gemäß Beispiel 1 verwendet, in der Nonenoylbernsteinsäureanhydrid durch Acetyltriethylcitrat (ATEC) ersetzt wurde. Zum Vergleich wurde eine Wäsche nur mit dem Waschmittel Dash gewaschen.
Waschversuche mit Formulierung: | 1 | Vergleichsbeispiel | Dash |
Anschmutzung: | |||
BW-gebleicht | 97,6 | 97,5 | 95,4 |
BW-Rotwein | 87,4 | 87,0 | 85,3 |
BW-Tee | 69,9 | 67,2 | 64,0 |
BW-Gras | 74,2 | 73,4 | 69,5 |
BW-Ketchup | 91,5 | 90,0 | 89,5 |
BW-Paprika | 56,0 | 55,6 | 53,1 |
Claims (5)
- Flüssige Bleichmittelsuspension bestehend im wesentlichen ausa) einer Mischung aus einem C8-C18-Fettalkohol, oxethyliert mit 1 bis 5 Einheiten Ethylenoxid, und einen C8-C18-Fettalkohol, oxethyliert mit 6 bis 25 Einheiten Ethylenoxid,b) einem cyclischen Anhydrid,c) einer wäßrigen Lösung von Wasserstoffperoxid undd) Wasser.
- Flüssige Bleichmittelsuspension nach Anspruch 1, dadurch gekennzeichnet, daß der Gehalt an oxethyliertem Fettalkohol a) 1 bis 50 Gew.-%, der Gehalt an cyclischem Anhydrid b) 0,5 bis 30 Gew.-%, der Gehalt an Wassestoffperoxid (100 %ig) 1 bis 30 Gew.-% und der Gehalt an Wasser bis zu 80 Gew.-% beträgt.
- Flüssige Bleichmittelsuspensionen nach Anspruch 1, dadurch gekennzeichnet, daß der pH-Wert der Suspension 2 bis 8 beträgt.
- Verwendung der flüssigen Bleichmittelsuspension als Komponente in Wasch- und Reinigungsmitteln.
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE19635070 | 1996-08-30 | ||
DE19635070A DE19635070A1 (de) | 1996-08-30 | 1996-08-30 | Flüssige Bleichmittelsuspension |
Publications (2)
Publication Number | Publication Date |
---|---|
EP0826770A2 true EP0826770A2 (de) | 1998-03-04 |
EP0826770A3 EP0826770A3 (de) | 1998-09-16 |
Family
ID=7804106
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP97114695A Withdrawn EP0826770A3 (de) | 1996-08-30 | 1997-08-25 | Flüssige Bleichmittelsuspension |
Country Status (3)
Country | Link |
---|---|
US (1) | US5916865A (de) |
EP (1) | EP0826770A3 (de) |
DE (1) | DE19635070A1 (de) |
Cited By (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO1999025801A1 (de) * | 1997-11-14 | 1999-05-27 | Henkel Kommanditgesellschaft Auf Aktien | Wässrige bleichmittel |
WO2013107579A1 (de) * | 2012-01-18 | 2013-07-25 | Henkel Ag & Co. Kgaa | Wasch-, reinigungs- oder vorbehandlungsmittel mit erhöhter reinigungskraft |
US11932833B2 (en) | 2021-02-18 | 2024-03-19 | The Clorox Company | Stable activated peroxide sanitizing liquid compositions without added phosphorous compounds or cationic surfactants |
Families Citing this family (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US20070167529A1 (en) * | 2006-01-17 | 2007-07-19 | Walton Rebecca A | Antimicrobial compositions for treating fabrics and surfaces |
Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
EP0497337A2 (de) * | 1991-02-01 | 1992-08-05 | Hoechst Aktiengesellschaft | Wässrige Suspensionen von Peroxicarbonsäuren |
JPH05156293A (ja) * | 1991-12-09 | 1993-06-22 | Kao Corp | 硬質表面用漂白洗浄剤組成物 |
EP0598170A1 (de) * | 1992-11-16 | 1994-05-25 | The Procter & Gamble Company | Reinigungs- und Bleichmittelzusammensetzungen |
Family Cites Families (30)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
NL113890C (de) * | 1955-07-27 | |||
NL239952A (de) * | 1959-06-19 | |||
US3996152A (en) * | 1975-03-27 | 1976-12-07 | The Procter & Gamble Company | Bleaching composition |
US4283301A (en) * | 1980-07-02 | 1981-08-11 | The Procter & Gamble Company | Bleaching process and compositions |
US4412934A (en) * | 1982-06-30 | 1983-11-01 | The Procter & Gamble Company | Bleaching compositions |
GR79230B (de) * | 1982-06-30 | 1984-10-22 | Procter & Gamble | |
GB8304990D0 (en) * | 1983-02-23 | 1983-03-30 | Procter & Gamble | Detergent ingredients |
GB2179669B (en) * | 1985-08-15 | 1988-12-29 | Procter & Gamble | Built liquid detergents |
EP0217454B1 (de) * | 1985-09-30 | 1992-03-11 | Unilever N.V. | Flüssige nichtwässrige Reinigungszusammensetzung und wasserfreies Perborat |
GB8527772D0 (en) * | 1985-11-11 | 1985-12-18 | Unilever Plc | Non-aqueous built liquid detergent composition |
US4806260A (en) * | 1986-02-21 | 1989-02-21 | Colgate-Palmolive Company | Built nonaqueous liquid nonionic laundry detergent composition containing acid terminated nonionic surfactant and quarternary ammonium softener and method of use |
US4772290A (en) * | 1986-03-10 | 1988-09-20 | Clorox Company | Liquid hydrogen peroxide/peracid precursor bleach: acidic aqueous medium containing solid peracid precursor activator |
DE3774312D1 (de) * | 1986-03-31 | 1991-12-12 | Procter & Gamble | Fluessige reinigungsmittel, welche einen anionischen oberflaechenaktiven stoff, ein salz der bernsteinsaeure als gerueststoff und eine fettsaeure enthalten. |
US4790952A (en) * | 1986-08-14 | 1988-12-13 | The Clorox Company | Alkyl monoperoxysuccinic acid precursors and method of synthesis |
DE3709348A1 (de) * | 1987-03-21 | 1988-10-06 | Degussa | Peroxycarbonsaeure enthaltende waessrige bleichmittelsuspensionen, verfahren zu ihrer herstellung und ihre verwendung |
DE3709347A1 (de) * | 1987-03-21 | 1988-10-06 | Degussa | Peroxycarbonsaeure enthaltende waessrige bleichmittelsuspensionen, verfahren zu ihrer herstellung und ihre verwendung |
GB8806704D0 (en) * | 1988-03-21 | 1988-04-20 | Unilever Plc | Stable liquid bleach compositions |
US4824592A (en) * | 1988-03-25 | 1989-04-25 | Lever Brothers Company | Suspending system for insoluble peroxy acid bleach |
JP2551991B2 (ja) * | 1989-01-25 | 1996-11-06 | 花王株式会社 | カビ取り剤組成物 |
EP0396287A3 (de) * | 1989-05-04 | 1991-10-02 | The Clorox Company | Verfahren und Erzeugnis für ein verbessertes Bleichen unter in situ Bildung von Persäure |
EP0476212A1 (de) * | 1990-09-17 | 1992-03-25 | The Procter & Gamble Company | Flüssige Waschmittelzusammensetzung |
EP0517996B1 (de) * | 1991-06-14 | 1993-12-15 | The Procter & Gamble Company | Wasserstoffperoxid enthaltende stabile Bleichmittelzusammensetzungen |
JPH04371546A (ja) * | 1991-06-17 | 1992-12-24 | Tatsuro Kuratomi | ダイヤモンド系焼結体およびその製造法 |
DE69229957T2 (de) * | 1991-12-13 | 2000-04-13 | The Procter & Gamble Co., Cincinnati | Acylierte citratester als ausgangsstoffe für persäuren |
EP0629691B1 (de) * | 1993-06-09 | 1998-10-21 | The Procter & Gamble Company | Stabile wässrige nichtionische Tensideemulsionen |
US5409632A (en) * | 1992-11-16 | 1995-04-25 | The Procter & Gamble Company | Cleaning and bleaching composition with amidoperoxyacid |
EP0626693A3 (de) * | 1993-03-31 | 1995-03-22 | Sgs Thomson Microelectronics | Multiplex-Leseverstärker. |
EP0619368A1 (de) * | 1993-04-06 | 1994-10-12 | The Procter & Gamble Company | Konzentrierte flüssige Waschmittelzusammensetzungen |
ATE186324T1 (de) * | 1993-06-09 | 1999-11-15 | Procter & Gamble | Stabile wässrige nichtionische tensidemulsionen |
EP0686691B1 (de) * | 1994-06-10 | 2001-08-08 | The Procter & Gamble Company | Wässrige Emulsionen mit Aufhellern |
-
1996
- 1996-08-30 DE DE19635070A patent/DE19635070A1/de not_active Withdrawn
-
1997
- 1997-08-25 EP EP97114695A patent/EP0826770A3/de not_active Withdrawn
- 1997-08-29 US US08/929,320 patent/US5916865A/en not_active Expired - Fee Related
Patent Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
EP0497337A2 (de) * | 1991-02-01 | 1992-08-05 | Hoechst Aktiengesellschaft | Wässrige Suspensionen von Peroxicarbonsäuren |
JPH05156293A (ja) * | 1991-12-09 | 1993-06-22 | Kao Corp | 硬質表面用漂白洗浄剤組成物 |
EP0598170A1 (de) * | 1992-11-16 | 1994-05-25 | The Procter & Gamble Company | Reinigungs- und Bleichmittelzusammensetzungen |
Non-Patent Citations (3)
Title |
---|
DATABASE WPI Section Ch, Week 9037 Derwent Publications Ltd., London, GB; Class D22, AN 90-279352 XP002072204 & JP 02 196 896 A (KAO CORP) * |
DATABASE WPI Section Ch, Week 9306 Derwent Publications Ltd., London, GB; Class L02, AN 93-048170 XP002072203 & JP 04 371 546 A (KURAMOTO T) * |
PATENT ABSTRACTS OF JAPAN vol. 017, no. 554 (C-1118), 6.Oktober 1993 & JP 05 156293 A (KAO CORP), 22.Juni 1993, * |
Cited By (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO1999025801A1 (de) * | 1997-11-14 | 1999-05-27 | Henkel Kommanditgesellschaft Auf Aktien | Wässrige bleichmittel |
WO2013107579A1 (de) * | 2012-01-18 | 2013-07-25 | Henkel Ag & Co. Kgaa | Wasch-, reinigungs- oder vorbehandlungsmittel mit erhöhter reinigungskraft |
US11932833B2 (en) | 2021-02-18 | 2024-03-19 | The Clorox Company | Stable activated peroxide sanitizing liquid compositions without added phosphorous compounds or cationic surfactants |
Also Published As
Publication number | Publication date |
---|---|
EP0826770A3 (de) | 1998-09-16 |
US5916865A (en) | 1999-06-29 |
DE19635070A1 (de) | 1998-03-05 |
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