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EP0033018A2 - Mixtures of optical brighteners - Google Patents

Mixtures of optical brighteners Download PDF

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Publication number
EP0033018A2
EP0033018A2 EP80108264A EP80108264A EP0033018A2 EP 0033018 A2 EP0033018 A2 EP 0033018A2 EP 80108264 A EP80108264 A EP 80108264A EP 80108264 A EP80108264 A EP 80108264A EP 0033018 A2 EP0033018 A2 EP 0033018A2
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EP
European Patent Office
Prior art keywords
alkoxy
alkyl
oder
optionally substituted
aralkyl
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
EP80108264A
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German (de)
French (fr)
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EP0033018A3 (en
EP0033018B1 (en
Inventor
Guenther Dr.-Chem. Seybold
Magnus Rosenkranz
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BASF SE
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BASF SE
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    • DTEXTILES; PAPER
    • D06TREATMENT OF TEXTILES OR THE LIKE; LAUNDERING; FLEXIBLE MATERIALS NOT OTHERWISE PROVIDED FOR
    • D06LDRY-CLEANING, WASHING OR BLEACHING FIBRES, FILAMENTS, THREADS, YARNS, FABRICS, FEATHERS OR MADE-UP FIBROUS GOODS; BLEACHING LEATHER OR FURS
    • D06L4/00Bleaching fibres, filaments, threads, yarns, fabrics, feathers or made-up fibrous goods; Bleaching leather or furs
    • D06L4/60Optical bleaching or brightening
    • D06L4/65Optical bleaching or brightening with mixtures of optical brighteners

Definitions

  • Residues Y and Z are in addition to hydrogen z.
  • B OCH 3 , OC 2 H 5 , OC 3 H 7 , OC 4 H 9 , OC 2 H 4 OCH 3 , OC 2 H 4 OC 2 H 5 , OC 2 H 4 OC 3 H 7 , OC 2 H 4 OC 4 H 9 , OC 2 H 4 or OC 2 H 4 OC 2 H 4 OCH 3 .
  • R The same alkoxy radicals and the following groups are to be mentioned for R: CH 3 , C 2 H 5 , C 3 H 7 , C 4 H 9 , C 5 H 11 , C 6 H 13 , C 8 H 17 , C 10 H 21 , , C 2 H 4 CN, CH 2 -CHO, CH 2 CN, C 2 H 4 COOCH 3 , CH 2 -COOC 2 H 5 , CH 2 -COOC 4 H 9 , C 2 H 4 Cl, C 2 H 4 OCH 3 , C 2 H 4 OC 2 H 4 OCH 3 , (CH 2 -CH 2 -O) 2 C 2 H 5 , (C 2 H 4 -O) 3 C 4 H 9 , C 2 H 4 SO 2 CH 3 , CH 2 COCH 3 , CH 2 C 6 H 5 or C 2 H 4 C 6 H 5 .
  • the mixtures according to the invention are obtained either by jointly dispersing compounds of the formulas I and II in the stated mixing ratio or else by separate dispersing of the components and mechanical mixing.
  • Preferred mixing ratios are in the range from 10 to 90% of compounds of the formula I.
  • the optimum mixing ratio depends in each case on the type of the respective compounds of the brighteners mentioned under the formulas I and II. It can easily be determined by simple preliminary tests.
  • the mixtures according to the invention are particularly suitable for optically brightening textile materials made of linear polyesters, polyamides and acetyl cellulose.
  • the mixtures according to the invention can be applied to the textile material by known methods, for example by the exhaust process at 90-140 ° C. with or without addition of dyeing accelerators (carriers) or by the thermosol process at temperatures of 160-210 ° C.
  • the mixtures according to the invention are distinguished by very favorable dyeing behavior.
  • the advantage of the mixtures compared to the individual components can be seen in the fact that this gives an unexpected synergistic effect with regard to the degree of whiteness, i.e. mixtures according to the invention result in a higher degree of whiteness than would be expected when considering the proportions of the individual components. The same applies to the brilliance of the brightening.
  • Preferred blending ratios are in the range of about 70-90: 30-10 (I: II) when high degrees of whiteness are desired and in the range of 30-60: 70-40 (I: II) when high lightfastness is required arrives.
  • Polyester staple fiber fabric is washed as usual, dried and impregnated on a padder with an aqueous dispersion which contains 1 g / 1 of a mixture of the optical brighteners of the formula I. contains 90 parts I and 10 parts II in a mixing ratio.
  • the material is then squeezed out so that there is a moisture absorption of 60%.
  • the material thus sealed is then dried on a stenter frame at 100 ° C. for 2 minutes and then thermosolated at 190 ° C. for 30 seconds.
  • the whiteness of the lightened textile material determined according to Berger is 134.
  • Polyester fiber fabric is treated as described in Example 1 with an aqueous dispersion containing 1 g / 1 of a mixture of the optical brighteners of the formula I. and contains.

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  • Engineering & Computer Science (AREA)
  • Textile Engineering (AREA)
  • Detergent Compositions (AREA)
  • Coloring (AREA)

Abstract

Die Erfindung betrifft Mischungen zweier oder mehrerer optischer Aufheller, enthaltend 5 bis 95 % von Verbindungen der allgemeinen Formel I

Figure imga0001
und 95 bis 5 %von Verbindungen der allgemeinen Formel II
Figure imga0002
wobei

  • n die Zahlen 1, 2 oder 3,
  • Y Wasserstoff oder gegebenenfalls substituiertes Alkoxy,
  • Z gegebenenfalls substituiertes Alkoxy,
  • R gegebenenfalls substituiertes C1- bis C10 -Alkyl oder Alkoxy und die Reste
  • X unabhängig voneinander Fluor, Chlor, Brom, Wasserstoff, C1- bis C10-Alkyl, Aralkyl, Aryl, Carbonester, gegebenenfalls substituiertes Carbamoyl oder Sulfamoyl, Alkyl-, Alkenyl-, Aralkyl- oder Aryl- sulfonyl, Alkanoyl, Aroyl oder Cyan bedeuten, mit der Maßgabe, daß für X = CN und n = 1 der Substituent X in meta-oder para-Stellung steht.
The invention relates to mixtures of two or more optical brighteners containing 5 to 95% of compounds of the general formula I.
Figure imga0001
and 95 to 5% of compounds of general formula II
Figure imga0002
in which
  • n the numbers 1, 2 or 3,
  • Y is hydrogen or optionally substituted alkoxy,
  • Z optionally substituted alkoxy,
  • R optionally substituted C 1 to C 10 alkyl or alkoxy and the radicals
  • X independently of one another fluorine, chlorine, bromine, hydrogen, C 1 - to C 10 -alkyl, aralkyl, aryl, carbonyl ester, optionally substituted carbamoyl or sulfamoyl, alkyl, alkenyl, aralkyl or arylsulfonyl, alkanoyl, aroyl or cyan mean, with the proviso that for X = CN and n = 1 the substituent X is in the meta or para position.

Description

Die Erfindung betrifft Mischungen zweier oder mehrerer optischer Aufheller, enthaltend 5 bis 95 % von Verbindungen der allgemeinen Formel I

Figure imgb0001
und 95 bis 5 % von Verbindungen der allgemeinen Formel II
Figure imgb0002
wobei

  • n die Zahlen 1, 2 oder 3,
  • Y Wasserstoff oder gegebenenfalls substituiertes Alkoxy,
  • Z gegebenenfalls substituiertes Alkoxy,
  • R gegebenenfalls substituiertes C1- bis C10-Alkyl oder Alkoxy und die Reste
  • X unabhängig voneinander Fluor, Chlor, Brom,Wasserstoff, C1- bis C10-Alkyl, Aralkyl, Aryl, Carbonester, gegebenenfalls substituiertes Carbamoyl oder Sulfamoyl, Alkyl-, Alkenyl-, Aralkyl- oder Arylsulfonyl, Alkanoyl, Aroyl oder Cyan bedeuten, mit der Maßgabe, daß für X = CN und n = 1 der Substituent X in meta- oder para-Stellung steht.
The invention relates to mixtures of two or more optical brighteners containing 5 to 95% of compounds of the general formula I.
Figure imgb0001
and 95 to 5% of compounds of general formula II
Figure imgb0002
in which
  • n the numbers 1, 2 or 3,
  • Y is hydrogen or optionally substituted alkoxy,
  • Z optionally substituted alkoxy,
  • R optionally substituted C 1 to C 10 alkyl or alkoxy and the radicals
  • X independently of one another are fluorine, chlorine, bromine, hydrogen, C 1 - to C 10 -alkyl, aralkyl, aryl, carboxylic esters, optionally substituted carbamoyl or sulfamoyl, alkyl, alkenyl, aralkyl or arylsulfonyl, alkanoyl, aroyl or cyano, with the proviso that for X = CN and n = 1 the substituent X is in the meta or para position.

Reste Y und Z sind neben Wasserstoff z. B. OCH3, OC2H5, OC3H7, OC4H9, OC2H4OCH3, OC2H4OC2H5, OC2H4OC3H7, OC2H4OC4H9, OC2H4 oder OC2H4OC2H4OCH3.Residues Y and Z are in addition to hydrogen z. B. OCH 3 , OC 2 H 5 , OC 3 H 7 , OC 4 H 9 , OC 2 H 4 OCH 3 , OC 2 H 4 OC 2 H 5 , OC 2 H 4 OC 3 H 7 , OC 2 H 4 OC 4 H 9 , OC 2 H 4 or OC 2 H 4 OC 2 H 4 OCH 3 .

Für R sind die gleichen Alkoxyreste sowie folgende Gruppen zu nennen: CH3, C2H5, C3H7, C4H9, C5H11, C6H13, C8H17, C10H21,

Figure imgb0003
, C2H4CN, CH2-CHO, CH2CN,
Figure imgb0004
C2H4COOCH3, CH2-COOC2H5, CH2-COOC4H9,
Figure imgb0005
Figure imgb0006
C2H4Cl, C2H4OCH3, C2H4O-C2H4OCH3, (CH2-CH2-O)2C2H5, (C2H4-O)3C4H9, C2H4SO2CH3, CH2COCH3, CH2C6H5 oder C 2 H 4 C 6 H 5.The same alkoxy radicals and the following groups are to be mentioned for R: CH 3 , C 2 H 5 , C 3 H 7 , C 4 H 9 , C 5 H 11 , C 6 H 13 , C 8 H 17 , C 10 H 21 ,
Figure imgb0003
, C 2 H 4 CN, CH 2 -CHO, CH 2 CN,
Figure imgb0004
C 2 H 4 COOCH 3 , CH 2 -COOC 2 H 5 , CH 2 -COOC 4 H 9 ,
Figure imgb0005
Figure imgb0006
C 2 H 4 Cl, C 2 H 4 OCH 3 , C 2 H 4 OC 2 H 4 OCH 3 , (CH 2 -CH 2 -O) 2 C 2 H 5 , (C 2 H 4 -O) 3 C 4 H 9 , C 2 H 4 SO 2 CH 3 , CH 2 COCH 3 , CH 2 C 6 H 5 or C 2 H 4 C 6 H 5 .

Reste X sind neben den bereits einzeln genannten beispielsweise: COOCH3, COOC2H5, COOC3H7, COOC4H9, COOC6H13, COOC8H17, COOC2H4OCH3,

Figure imgb0007
, COOC10H21, COOC2H4OC2H5, COOC2H4OC4H9, COO(C2H4O)2CH3, CONH2, CONHCH3, CON(C2H5)2, CON(CH3)2,
Figure imgb0008
CONHC4H9 sowie die entsprechenden Sulfamoylreste, SO2CH3, SO2C2H5, SO2C4H9, SO2CH2-CH=CH2, SO2CH2C6H5, SO2C6H5, CH3CO, C2H5CO, C3H7CO, C4H9CO, C6H5CO2, CH2C6H5, C2H4C6H5, C5H5, C6H4CH3 oder C6H4Cl sowie die für R genannten Alkylreste. 'In addition to those already mentioned individually, radicals X are, for example: COOCH 3 , COOC 2 H 5 , COOC 3 H 7 , COOC 4 H 9 , COOC 6 H 13 , COOC 8 H 17 , COOC 2 H 4 OCH 3 ,
Figure imgb0007
, COOC 10 H 21 , COOC 2 H 4 OC 2 H 5 , COOC 2 H 4 OC 4 H 9 , COO (C 2 H 4 O) 2 CH 3 , CONH 2 , CONHCH 3 , CON (C 2 H 5 ) 2 , CON (CH 3 ) 2 ,
Figure imgb0008
CONHC 4 H 9 and the corresponding sulfamoyl radicals, SO 2 CH 3 , SO 2 C 2 H 5 , SO 2 C 4 H 9 , SO 2 CH 2 -CH = CH 2 , SO 2 CH 2 C 6 H 5 , SO 2 C 6 H 5 , CH 3 CO, C 2 H 5 CO, C 3 H 7 CO, C 4 H 9 CO, C 6 H 5 CO 2 , CH 2 C 6 H 5 , C 2 H 4 C 6 H 5 , C 5 H 5 , C 6 H 4 CH 3 or C 6 H 4 Cl and the alkyl radicals mentioned for R. '

Die erfindungsgemäßen Mischungen erhält man entweder durch gemeinsames Dispergieren von Verbindungen der Formeln I und II im angegebenen Mischungsverhältnis oder aber durch getrenntes Dispergieren der Komponenten und mechanisches Mischen. Bevorzugte Mischungsverhältnisse liegen im Bereich von 10 bis 90 % von Verbindungen der Formel I. Das optimale Mischungsverhältnis hängt im Einzelfall von der Art der jeweiligen Verbindungen der unter den Formeln I und II genannten Aufheller ab. Es läßt sich unschwer durch einfache Vorversuche ermitteln.The mixtures according to the invention are obtained either by jointly dispersing compounds of the formulas I and II in the stated mixing ratio or else by separate dispersing of the components and mechanical mixing. Preferred mixing ratios are in the range from 10 to 90% of compounds of the formula I. The optimum mixing ratio depends in each case on the type of the respective compounds of the brighteners mentioned under the formulas I and II. It can easily be determined by simple preliminary tests.

Die erfindungsgemäßen Mischungen eignen sich besonders zum optischen Aufhellen von Textilmaterialien aus linearen Polyestern, Polyamiden und von Acetylcellulose. Die erfindungsgemäßen Mischungen können nach bekannten Methoden auf das Textilgut appliziert werden, so beispielsweise nach dem Ausziehverfahren bei 90 - 140°C mit oder ohne Zusatz von Färbebeschleunigern (Carriern) oder nach dem Thermosolverfahren bei Temperaturen von 160 - 210°C.The mixtures according to the invention are particularly suitable for optically brightening textile materials made of linear polyesters, polyamides and acetyl cellulose. The mixtures according to the invention can be applied to the textile material by known methods, for example by the exhaust process at 90-140 ° C. with or without addition of dyeing accelerators (carriers) or by the thermosol process at temperatures of 160-210 ° C.

Die erfindungsgemäßen Mischungen zeichnen sich durch sehr günstiges färberisches Verhalten aus. Der Vorteil der Mischungen im Vergleich zu den Einzelkomponenten ist darin zu sehen, daß man damit einen unerwarteten synergistischen Effekt in Bezug auf den Weißgrad erhält, d.h., erfindungsgemäße Mischungen ergeben einen höheren Weißgrad als unter Berücksichtigung der Anteile der Einzelkomponenten zu erwarten wäre. Das gleiche gilt für die Brillanz der Aufhellungen.The mixtures according to the invention are distinguished by very favorable dyeing behavior. The advantage of the mixtures compared to the individual components can be seen in the fact that this gives an unexpected synergistic effect with regard to the degree of whiteness, i.e. mixtures according to the invention result in a higher degree of whiteness than would be expected when considering the proportions of the individual components. The same applies to the brilliance of the brightening.

Von besonderer Bedeutung sind Mischungen von Verbindungen der Formel I und II, bei denen

  • X Cyan, Chlor, Carbonester oder Alkyl,
  • R C1- bis C8-Alkyl oder Formyl-C1- bis C3-alkyl,
  • Y Wasserstoff, C1- bis C4-Alkoxy oder C1- bis C4-Alkoxy-C1- bis C4-alkoxy und
  • Z C1- bis C4-Alkoxy oder C1- bis C4-Alkoxy-C1- bis C4- alkoxy sind.
Mixtures of compounds of the formula I and II in which
  • X cyan, chlorine, carboxylic ester or alkyl,
  • RC 1 to C 8 alkyl or formyl C 1 to C 3 alkyl,
  • Y is hydrogen, C 1 to C 4 alkoxy or C 1 to C 4 alkoxy-C 1 to C 4 alkoxy and
  • ZC 1 to C 4 alkoxy or C 1 to C 4 alkoxy-C 1 to C 4 alkoxy.

Bevorzugte Mischungsverhältnisse liegen im Bereich von ungefähr 70 - 90 : 30 - 10 (I : II), wenn hohe Weißgrade .erwünscht sind, und im Bereich von 30 - 60 : 70 - 40 (I : II), wenn es auf eine hohe Lichtechtheit ankommt.Preferred blending ratios are in the range of about 70-90: 30-10 (I: II) when high degrees of whiteness are desired and in the range of 30-60: 70-40 (I: II) when high lightfastness is required arrives.

In den folgenden Beispielen beziehen sich Angaben über Teile und Prozente, sofern nicht anders vermerkt, auf das Gewicht.In the following examples, parts and percentages are by weight unless otherwise noted.

Die Weißgrade wurden nach Berger (Die Farbe, 8 (1959), S 187 ff) gemessen.The degrees of whiteness were measured according to Berger (Die Farbe, 8 (1959), S 187 ff).

Beispiel 1example 1

Polyesterstapelfasergewebe wird wie üblich gewaschen, getrocknet und auf einem Foulard mit einer wäßrigen Dispersion imprägniert, die 1 g/1 einer Mischung der optischen Aufheller der Formel I

Figure imgb0009
Figure imgb0010
im Mischungsverhältnis 90 Teile I und 10 Teile II enthält.Polyester staple fiber fabric is washed as usual, dried and impregnated on a padder with an aqueous dispersion which contains 1 g / 1 of a mixture of the optical brighteners of the formula I.
Figure imgb0009
Figure imgb0010
contains 90 parts I and 10 parts II in a mixing ratio.

Das Material wird dann so abgequetscht, daß sich eine Feuchtigkeitsaufnahme von 60 % ergibt. Das so geklotzte Material wird anschließend auf einem Spannrahmen 2 Minuten bei 100°C getrocknet und dann 30 sec bei 190°C thermosoliert. Der nach Berger ermittelte Weißgrad des so aufgehellten Textilmaterials beträgt 134.The material is then squeezed out so that there is a moisture absorption of 60%. The material thus sealed is then dried on a stenter frame at 100 ° C. for 2 minutes and then thermosolated at 190 ° C. for 30 seconds. The whiteness of the lightened textile material determined according to Berger is 134.

Wenn man Verbindungen der Formel I

Figure imgb0011
mit Verbindungen der Formel II
Figure imgb0012
im in der folgenden Tabelle angegebenen Verhältnis mischt, erhält man ebenfalls sehr gute Aufhellungen:
Figure imgb0013
If compounds of the formula I
Figure imgb0011
with compounds of formula II
Figure imgb0012
mixed in the ratio given in the following table, you also get very good lightenings:
Figure imgb0013

Beispiel 11Example 11

Polyesterfasergewebe wird wie in Beispiel 1 beschrieben mit einer wäßrigen Dispersion behandelt, die 1 g/1 einer Mischung der optischen Aufheller der Formel I

Figure imgb0014
Figure imgb0015
und
Figure imgb0016
enthält.Polyester fiber fabric is treated as described in Example 1 with an aqueous dispersion containing 1 g / 1 of a mixture of the optical brighteners of the formula I.
Figure imgb0014
Figure imgb0015
and
Figure imgb0016
contains.

Man erhält so eine brillante Weißaufhellung.This gives a brilliant white lightening.

Claims (3)

1. Mischungen zweier oder mehrerer optischer Aufheller, enthaltend 5 bis 95 % von Verbindungen der allgemeinen Formel I
Figure imgb0017
und 95 bis 5 % von Verbindungen der allgemeinen Formel II
Figure imgb0018
wobei n die Zahlen 1, 2 oder 3, Y Wasserstoff oder gegebenenfalls substituiertes Alkoxy, Z gegebenenfalls substituiertes Alkoxy, R gegebenenfalls substituiertes C1- bis C10-Alkyl oder Alkoxy und die Reste X unabhängig voneinander Fluor, Chlor, Brom, Wasserstoff, C1- bis C10-Alkyl, Aralkyl, Aryl, Carbonester, gegebenenfalls substituiertes Carbamoyl oder Sulfamoyl, Alkyl-, Alkenyl-, Aralkyl- oder Arylsulfonyl, Alkanoyl, Aroyl oder Cyan bedeuten, mit der Maßgabe, daß für X = CN und n = 1 der Substituent X in meta- oder para-Stellung steht.
1. Mixtures of two or more optical brighteners containing 5 to 95% of compounds of general formula I.
Figure imgb0017
and 95 to 5% of compounds of general formula II
Figure imgb0018
in which n the numbers 1, 2 or 3, Y is hydrogen or optionally substituted alkoxy, Z optionally substituted alkoxy, R optionally substituted C 1 -C 10 -alkyl or alkoxy and the radicals X independently of one another are fluorine, chlorine, bromine, hydrogen, C 1 - to C 10 -alkyl, aralkyl, aryl, carboxylic esters, optionally substituted carbamoyl or sulfamoyl, alkyl, alkenyl, aralkyl or arylsulfonyl, alkanoyl, aroyl or cyano, with the proviso that for X = CN and n = 1 the substituent X is in the meta or para position.
2. Mischungen gemäß Anspruch 1, bei denen X Cyan, Chlor, Carbonester oder Alkyl, R C1- bis C8-Alkyl oder Formyl-C1- bis C3-alkyl, Y Wasserstoff, C1- bis C4-Alkoxy oder C1- bis C4-Alkoxy-C1- bis C4-alkoxy und Z C1- bis C4-Alkoxy oder C1- bis C4-Alkoxy-C1- bis C4-alkoxy sind. 2. Mixtures according to claim 1, in which X cyan, chlorine, carboxylic ester or alkyl, RC 1 to C 8 alkyl or formyl C 1 to C 3 alkyl, Y is hydrogen, C 1 to C 4 alkoxy or C 1 to C 4 alkoxy-C 1 to C 4 alkoxy and ZC 1 to C 4 alkoxy or C 1 to C 4 alkoxy-C 1 to C 4 alkoxy. 3. Verwendung der Mischungen gemäß Anspruch 1 oder 2 als optische Aufheller für Polyester, Polyamide oder Celluloseester.3. Use of the mixtures according to claim 1 or 2 as optical brighteners for polyesters, polyamides or cellulose esters.
EP80108264A 1980-01-12 1980-12-31 Mixtures of optical brighteners Expired EP0033018B1 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE19803001066 DE3001066A1 (en) 1980-01-12 1980-01-12 MIXTURES OF OPTICAL BRIGHTENERS
DE3001066 1980-01-12

Publications (3)

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EP0033018A2 true EP0033018A2 (en) 1981-08-05
EP0033018A3 EP0033018A3 (en) 1981-08-12
EP0033018B1 EP0033018B1 (en) 1985-04-10

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JP (1) JPS56104981A (en)
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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0252009A1 (en) * 1986-07-01 1988-01-07 Ciba-Geigy Ag 1,4-Distyryl benzene compounds and their mixtures with other 1,4-distyryl benzene compounds
WO1999005356A1 (en) * 1997-07-25 1999-02-04 Clariant Gmbh Mixtures of optical brighteners

Family Cites Families (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2929591A1 (en) * 1979-07-21 1981-02-05 Hoechst Ag MIXTURES OF OPTICAL BRIGHTENERS

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0252009A1 (en) * 1986-07-01 1988-01-07 Ciba-Geigy Ag 1,4-Distyryl benzene compounds and their mixtures with other 1,4-distyryl benzene compounds
WO1999005356A1 (en) * 1997-07-25 1999-02-04 Clariant Gmbh Mixtures of optical brighteners
US6120704A (en) * 1997-07-25 2000-09-19 Clariant Gmbh Mixtures of optical brighteners

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Publication number Publication date
EP0033018A3 (en) 1981-08-12
EP0033018B1 (en) 1985-04-10
JPS56104981A (en) 1981-08-21
DE3001066A1 (en) 1981-07-16
DE3070492D1 (en) 1985-05-15

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