CA1109063A - Azo dyes, processes for producing them, and their use - Google Patents

Azo dyes, processes for producing them, and their use

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Publication number
CA1109063A
CA1109063A CA299,037A CA299037A CA1109063A CA 1109063 A CA1109063 A CA 1109063A CA 299037 A CA299037 A CA 299037A CA 1109063 A CA1109063 A CA 1109063A
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CA
Canada
Prior art keywords
formula
alkoxy
process according
azo dye
cyano
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
Application number
CA299,037A
Other languages
French (fr)
Inventor
Peter Aeschlimann
Stefan Koller
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.)
BASF Schweiz AG
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Individual
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
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Publication of CA1109063A publication Critical patent/CA1109063A/en
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Classifications

    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09BORGANIC DYES OR CLOSELY-RELATED COMPOUNDS FOR PRODUCING DYES, e.g. PIGMENTS; MORDANTS; LAKES
    • C09B29/00Monoazo dyes prepared by diazotising and coupling
    • C09B29/06Monoazo dyes prepared by diazotising and coupling from coupling components containing amino as the only directing group
    • C09B29/08Amino benzenes
    • C09B29/0805Amino benzenes free of acid groups
    • C09B29/0807Amino benzenes free of acid groups characterised by the amino group
    • C09B29/0809Amino benzenes free of acid groups characterised by the amino group substituted amino group
    • C09B29/0811Amino benzenes free of acid groups characterised by the amino group substituted amino group further substituted alkylamino, alkenylamino, alkynylamino, cycloalkylamino aralkylamino or arylamino
    • C09B29/0813Amino benzenes free of acid groups characterised by the amino group substituted amino group further substituted alkylamino, alkenylamino, alkynylamino, cycloalkylamino aralkylamino or arylamino substituted by OH, O-C(=X)-R, O-C(=X)-X-R, O-R (X being O,S,NR; R being hydrocarbonyl)
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09BORGANIC DYES OR CLOSELY-RELATED COMPOUNDS FOR PRODUCING DYES, e.g. PIGMENTS; MORDANTS; LAKES
    • C09B29/00Monoazo dyes prepared by diazotising and coupling
    • C09B29/0003Monoazo dyes prepared by diazotising and coupling from diazotized anilines

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Coloring (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

Abstract

Abstract of the Disclosure New disperse azo dyes are disclosed which correspond to the formula

Description

1~39~ 3 The invention relates to new azo dyes of the disperse class, to processes for producing them, and to their use for dyeing and printing synthetic fibres, especially fibres containing ester groups, particularly polyester materials.
The new azo dyes free from water-solubilising groups correspond to the formula /N2 ORl ~ /~
02N~ ~-- N----N ~ NH - CH2 - CH - R2 \~ ~/ OH

wherein Xrepresents halogen, Rl represents unsubstituted alkyl, alkyl which is substituted by halogen, cyano, aIkoxy or ~-alkoxy ethylene, wherein the aIkoxy-part may be further substituted by cyano or cycloalkyl, '- R2 represents unsubstituted lower aIkyl, and R3 represents unsubstituted lcwer alkyl or lower alkyl which may be sub-- stituted by halogen, cyano or alkoxy.
In preferred azo dyes, X represents chlorine, Rl represents an aIkyl group which has 1 to 3 carbon atcms and which is substituted by chlorine, cyano, methoxy or ethoxy, and especially the group -CH2CH2OR4 in which R4 represents methyl or ethyl, and R2 and R3 independently of one another each represent methyl or ethyl.
- 2 -- ' ' ~1~9~3 Preferred azo dyes are those of the formula N02 ORl"

02N - ~ N=N ~ Nl - C~12 - I1 2 OH
Hal 3 - 2a -~9~

wherein Hal represents chlorine or bromine, Rl" represents branched-chain or substituted alkyl, R2 represents unsubstituted lower alkyl, and R3" represents methyl, ethyl or propyl, which can be optionally substituted with halogen, particularly chlorine.
Particularly valuable dyes are those of the formula ~2 ~Rl"
02N ~ N = N ~ NH-CH2-CH-(CH3, C2H
OH
(Br, Cl) NHCO-(CH3, C2H5) wherein Rl" has the same meaning as above, especially -CH2CH20CH3 and CH(CH3)2-In the above formulae, Rl" represents in particular abranched-chain alkyl group, or an alkyl group substituted by ether groups, and R2 and R3 independently of one another represent methyl or ethyl.
Suitable groups Rl and/or R3 are, for example, those of the ( 3)2~ CH2CH2Cl, -CH2CH2Br, -CHCl-CH2Cl -cH2cH2cN, -cH2-cH(OH)-cH2cl~ -CH2c6H5~ -CH2C6H4N02~ -CH2c6H4 -CH2CH2C6H5, -CH2CH20H, -CH2CH2-0-CH3, -CH2CH2-0-C4Hg -C4H8-o-c4H9~ -CH2CH2-0-cH2cH20cH3~ -CH2CH2-0-CH2CH2-OH~
-C H -CH -CH2CH2-0-CH2CH2-0COCH3' -CH2CH2-0-CH2CH2-CN' -CH2-CH2-0-COCH2Cl, -CH2CH2-0-CO-CHBr-CH2Br, -CH2-CH-(GCOCH3)-CH2-0-C6H5, -CH2-CH2-0-CO-CH=CH2, -cH2-cH(OcOcH3)-cH2ococH3 -(CH2)1-3--CO(H' CH3~ C2H5' C3H7 4 9)' (CH2)1-3-~H-cO(H~ CH3, C2H5, C3H7, C4H ) -(CH2)l_3-o-co(c6H5~ C6H4Cl, C6H4Br, C5H40CH3, C6H4CH3), -(CH2)1-3-0-CO-O(cH3. C2H5, C3H7, C4H9), '~
, -(CH2)1_3-0-CO-O-(C6H5, C6~14Cl, C6H4Br, C6H40CH3, C6H4CH3)~
-CH2CH2-0-C6H5 und -CH2CH2-0-CO-C~12-C6H5.
Lower alkyl groups in the present description are taken to be groups having 1 to 5 carbon atoms; and branched-chain alkyl is in particular isopropyl.
These azo dyes are obtained by coupling coupling components of the formula ORl ~: ~HCOR3 OH
. . .
wherein Rl, R2 and R3 have the same meaning as above, with the diazonium compound of a 2,4-dinitro-6-halogenoaniline of the : formula . ~0 $i O~N ~ NH2 wherein X has the same meaning as above.
The coupling components of the given formula are obtained by reaction of an amine of the formula , ORl with an epoxide of the formula ` CH - CH - R
~-: \20 / 2 whereby there are obtained, in addition to the main product '. of the formula , ~ - 4 -.

. . .

C9~

Ç~

or its isomers of the formula OR
-CH-CH -OH
~=~ , 2 N~ICOR3 R2 also bis-addition products together with a small amount of unreacted starting amine as a mixture.
The new water-insoluble azo dyes, their mixtures with each other and mixtures thereof with other azo dyes, are excellently suitable for dyeing and printing leather, wool, silk and, in particular, synthetic fibres, such as acrylic fibres or acrylo-nitrile fibres, from polyacrylonitrile, or copolymers from ,. . .
~^ - acrylonitrile and other vinyl compounds, such as acrylic esters, acrylic amides, vinylpyridine, vinyl chloride or vinylidene chloride, or from copolymers of dicyanoethylene and vinyl acetate, ' and also acrylonitrile-block copolymers, fibres from polyurethanes, , polypropylene fibres, especially from polypropylene fibres modified with metals, particularly with nickel, from cellulose s tri- and -2 1/2~acetate, and especially fibres from polyamides,` such as nylon-6, nylon-6.6 or nylon 12, and from aromatic ' polyesters, such as those from terephthalic acid and ethylene glycol or 1,4-dimethylcyclohexane, and copolymers from terephthalic ~ ~9~~

acid and isophthalic acid and ethylene glycol.
The present invention relates also to a process for dyeing and printing textile material based on synthetic fibres, in particular on polyester fibres, in which process there are used azo dyes which are free from water-solubilising groups and which correspond to the formula N02 ~ORl 02N ~ N = N ~ NH-CH2-CH-R2 / OH

wherein X, Rl, R2 and R3 have the same meanings as above.
For dyeing in aqueous liquors, the water-insoluble dyes according to the present invention are used advantageously in a finely divided form, and dyeing is performed with the addition of dispersing agents, such as sulphite cellulose liquor or synthetic detergents, or a combination of various wetting and dispersing agents. It is as a rule expedient to convert before dyeing the dyes to be used into a dye preparation containing a dispersing agent and finely divided dye in such a form that a fine dispersion is obtained on dilution of the dye preparations with water. Such dye preparations can be produced in a known manner, for example by grinding the dye in dry or wet form, with or without the addition of dispersing agents during the grinding operation.
To obtain strong dyeings on polyethylene terephthalate fibres, it proves advantageous to add a swelling agent to the ',,-,. , ~3'9~

dye bath; or to perform the dyeing process under pressure at temperatures above 100C, for example at 130C. Suitable swelling agents are aromatic carboxylic acids, for example salicylic acid, phenols, such as o- or p-oxydiphenyl, or aromatic halogen compounds, such as o-dichlorobenzene or diphenyl.
For thermofixing the dye, the padded polyester fabric is heated, advantageously after prior drying, e.g. in a warm stream of air, at temperatures of above 100C, for example between 180 and 210C.
The dyeings obtained according to the present process can be subjected to an aftertreatment, for example by heating in an aqueous solution of an ion-free detergent.
The stated dyes can be applied according to the present process not only by impregnation but also by printing. For this purpose there is used, for example, a printing paste which contains the finely dispersed dye together with the auxiliaries customarily used in printing, such as wetting and thickening agents.
Full dyeings and printing having good fastness properties are obtained by the present process.
Full dyeings are likewise obtained with application of the new dyes from organic solvents, where the dye is applied from a solvent, in which it is dissolved or is present as a fine dispersion, to the textile article to be dyed. Suitable solvents are, e.g., petroleum fractions and, in particular, chlorinated hydrocarbons (e.g. perchloroethylene), which can be used on their 9.~

own, or as a dispersion together with water.
The new water-insoluble dyes can be used also for the solution dyeing of polyamides, polyesters and polyolefins.
The polymer to be dyed is advantageously mixed in the form of powders, granules or chips, as a finished spinning solution or in the melted state, with the dye, which is introduced in the dry condition or in the form of a dispersion or solution in an optionally volatile solvent. After homogeneous dispersion of the dye in the solution or melt of the polymer, the mixture is processed in a known manner, by casting, moulding or extrusion, into the form of fibres, yarns, monofilaments, films, and so forth.
The new dyes are suitable also for the so-called transfer or sublimation printing process, in which the dye is sublimated in the hot state from an auxiliary carrier (e.g. paper) onto the sheet material to be printed (e.g. made from polyester fibres).
Except where otherwise stated in the Examples which follow, parts are parts by weight, percentages are per cent by weight, and temperatures are in degrees Centigrade.

" ~ .
.

Example 1 21.75 g of 2,4-dinitro-6-chloroaniline is suspended in 50 ml of H2S04 (88%), and 16.8 ml of a 40% nitrosylsulphuric acid is added at 10-15 in the course of 30 minutes. After 3 hours, the clear diazo solution is added dropwise to a clear acidified solution of 43.6 g of the coupling component of the formula ~ Or~H2CH20CH3 H2-cH3 I OH

in 200 ml of ice water, the temperature being held below 5 by the addition of ice.
A pH value of about 3 is obtained by the simultaneous dropwise addition of conc. sodium hydroxide solution. The resulting dye of the formula 02N ~ N=N ~ _ NU-CH2-clu-cH2 3 is filtered off, and washed with hot water until the filtrate is colourless. After drying, there remains 50 g of a navy blue powder. The dye produces on polyester fabrics deeply coloured blue dyeings having good fastness to light and to sublimation.
The coupling component uséd in this Example is obtained by reacting the amine of the formula -- g _ ~ .

~ 9 OC21140C~H3 Ç~_ NH2 ..

at 20 - 30 in glacial acetic acid, with an equimolar amount of 1,2-butylene oxide.

Example 2 21.75 g of 2,4-dinitro-6-chloroaniline is diazotised as described in Example 1. The diazo solution is added dropwise to a solution consisting of 40 g of a coupling component of the formula IOC~(CH3)2 CH2 ~CH CH2-CH3 ~: l H

. NHCOCH3 dissolved in 200 ml of ice water and 12 parts by volume of conc.

hydrochloric acid. The resulting dye of the formula Cl OCH(CH3)2 02N ~ N=N ~ ~ - NH-CH2-~H-CH -CH

N2. NHCOCH3 is filtered off and washed with hot water. After drying, there is obtained 51 g of a navy blue dye which, applied in the HT process to polyester fabric, is distinguished by very good - fastness properties, and also by a high rate of absorption.

The coupling component is obtained by addition of equimolar amounts of 1,2-butylene oxide to the amine of the formula OCH(CH3)2 Example 3 The dye of the formula Cl OCH2CH20CH3 o2N~<$N=N ~ NH- CU2 - CII- CH2- C1:3 NO2 NHCOCH2CH3 . OH
; is obtained in a manner analogous to that described in Example 1 by using, in place of the coupling component described in Example 1, 32.5 g of the coupling component of the formula : ~ ~H-cH2-fH-cH2-CH3 OH

There is obtained 51 g of a navy blue disperse dye having very good build-up properties on polyester fabrics.

In an analogous manner are obtained the dyes of the formula X ORl .
02N~N=N~ f which likewise dye polyester fabrics in deep navy blue shades.

9~

__ ~ t No. X Rl R2 3 _ 21 Cl -CH(CH3)2 _CC231~ CH2CH3 4 ll ll ll -CH3Cl " . -CH2CH2Cl 6 ll ll -c2~5 "
7 ll .. ll -CH2 8 Br .. ll ll 11 . . -C"H3 CH2CH2Cl 12 l . , CC235 -CH3 14 . l . CH2CH3 ll ll -C2~lS "
16 Cl -CH2CH20CH3 -CH -CH3 17 .l l .l -CH2CH3 18 Br 19 . ll C2H,5 ll ll -CH3 .
21 ll ll -CH3 ll 22 ~l l CH2Cl 23 ll ll ll -CH2CH2Cl 24 l l C2H5 "
" ll . " -CH2 26 Cl " .. ll ll 27 ll ll ll -CH2CH2Cl .
28 . " . -CH
29 ll ll " -CH2 Cl -CH2CH(CH3)2 -C2~15 -CH3 ' . _ . . _ . - 13 - _ .__ "';

: ~ .
- ~

- --~ - ~
No. X R.l R2 R3 .' ~
; 31 Br -CH3 C2H5 -CH3 .i 3323 .l CH2C 20CH2CH3 A C1~2CH3 . 34 ll ll ll -CH2 . 35 ll ll -CH3 -CH3 ( 36 ll ll ll CCHH2CH13 " 39 Cl . "C2H5 CH23CH3 ll ll ll -CH2 ' 41 ll ll -.CH3 -CH3 42 ,l. Il ,l CH2CH3 . 43 ll ll ll -CH2 : 44 Cl -cH2cH2ocH(cH3)2 ,l -CH3 i 45 ll ll ll -CH2CH3 .~ 46 ll ~l ll -CH2Cl 47 Br ~l ll -CH .
!: 48 ll It . '' CcH3cHl3 ' Sl ll ll - "C2H5 CHH32CH3 . ' - . S2 ,l l l -CH2Cl ,.~ 53 Cl ~ ~ C 2 3 .~ 56 Cl -~H2cH2ocH2cH2c~l2cH3 - " -CH3 57 ll . Il ll -CH2CH3 . S8 Br l l CCHH23CH3 - 60 Cl - CH(CH3)2 -CH3 CH2CH2C 3 ;
~ - 14 -. . .

. . , . . . . ~

No. _ _ _ _ 2 _ _ 61 Cl- C~l(C113)2 -C2H5 -CH2C~2C~1 62 Br ll ll ..
63 ,l l -C113 64 Cl~ CH2CH20CH3 l l .l " C2H5 "
66 Br ll " .
67 ll ll -CH3 ll 68 Cl " . ll -CH(CH3)2 69 .l-CH2CH20CH2CH2CN C2H5 CH3 ll ~. I ., -C~12CH3 71 ,l-CH2CH2CN l . -72 " ll ll -C~3 73 ll ll -C~
74 l -CH2CH2Cl C2H5 l I~ .l .l CH2CH3 76 ll ~ -CH3 -CH3 77 .l .l l CH2CH3 78 l l l -CH2C
79 . -CH3 l -CH2CH2C
ll ll C2H5 -CH3 81 ll ll ll . -CH2CH3 82 - . l : -CH2CH2C
83 ll . ll -CH2 84 Br ll ll j, ll ~, . -CH2CH3 86 .. -CH2Cl ¦
., ~ .

.
.
~ 15 -

Claims (40)

THE EMBODIMENTS OF THE INVENTION IN WHICH AN EXCLUSIVE
PROPERTY OR PRIVILEGE IS CLAIMED ARE DEFINED AS FOLLOWS:
1. An azo dye of the formula wherein X represents halogen, R1 represents unsubstituted alkyl, alkyl which is substituted by halogen, cyano, alkoxy or .beta.-alkoxy ethylene, wherein the alkoxy-part may be further substituted by cyano or cycloalkyl, R2 represents unsubstituted lower alkyl, and R3 represents unsubstituted lower alkyl or lower alkyl which may be substituted by halogen, cyano or alkoxy.
2. An azo dye according to claim 1 wherein X represents chlorine.
3. An azo dye according to claim 1 wherein R1 represents alkyl which is substituted by halogen, cyano, alkoxy or .beta.-alkoxy ethylene, wherein the alkoxy-part may be further substituted by cyano.
4. An azo dye according to claim 3 wherein R1 represents an alkyl group which has 1 to 3 carbon atoms and which is substitut-ed by chlorine, cyano, methoxy or ethoxy.
5. An azo dye according to claim 4 wherein R1 represents the group -CH2-CH2-O-R4, in which R4 represents methyl or ethyl.
6. An azo dye according to claim 1 wherein R2 represents methyl or ethyl.
7. An azo dye according to claim 1 wherein R3 represents methyl or ethyl.
8. An azo dye which corresponds to the formula wherein Hal represents chlorine or bromine, R1" represents branched-chain alkyl or alkyl which is sub-stituted by halogen, cyano, alkoxy or ?-alkoxy ethylene, wherein the alkoxy-part may be further substituted by cyano, R2 represents unsubstituted lower alkyl, and R3" represents methyl, ethyl or propyl, which can be optionally substituted with halogen.
9. An azo dye according to claim 8 wherein R3" represents methyl, ethyl or propyl substituted with chlorine.
10. An azo dye which corresponds to the formula wherein R1" has the same meaning as in claim 8.
11. An azo dye which corresponds to the formula
12. An azo dye which corresponds to the formula
13. An azo dye which corresponds to the formula
14. An azo dye which corresponds to the formula
15. An azo dye which corresponds to the formula
16. An azo dye which corresponds to the formula
17. An azo dye which corresponds to the formula
18. An azo dye which corresponds to the formula
19. A process for producing azo dyes of the formula wherein X represents halogen, R1 represents unsubstituted alkyl, alkyl which is substituted by halogen, cyano, alkoxy or .beta.-alkoxy ethylene, wherein the alkoxy-part may be further substituted by cyano, or cyclo-alkyl, R2 represents unsubstituted lower alkyl, and R3 represents unsubstituted lower alkyl or lower alkyl which may be substituted by halogen, cyano or alkoxy, in which process coupling components of the formula wherein R1, R2 and R3 have the same meaning as above, are coupled with the diazonium compound of a 2,4-dinitro-6-halogeno-aniline of the formula wherein X has the same meaning as above.
20. A process according to claim 19 wherein there is used a diazonium compound in which X represents chlorine or bromine.
21. A process according to claim 19 wherein there is used a coupling component in which R1 represents alkyl which is sub-stituted by halogen, cyano, alkoxy or .beta.-alkoxy ethylene, wherein the alkoxy-part may be further substituted by cyano.
22. A process according to claim 21 wherein there is used a coupling component in which R1 represents an alkyl group which has 1 to 3 carbon atoms and which is substituted by chlorine, cyano, methoxy or ethoxy.
23. A process according to claim 22 wherein there is used a coupling component in which R1 represents the group of the formula -CH2CH2OR4, wherein R4 represents methyl or ethyl.
24. A process according to claim 19 wherein there is used a coupling component in which R2 represents methyl or ethyl.
25. A process according to claim 19 wherein there is used a coupling component in which R3 represents methyl or ethyl.
26. A process according to claim 19 wherein there is used a coupling component of the formula in which R1" represents branched-chain alkyl or alkyl which is substituted by halogen, cyano, alkoxy or .beta.-alkoxy ethylene, wherein the alkoxy-part may be further substituted by cyano, R2 represents unsubstituted lower alkyl, and R3" represents methyl, ethyl or propyl which can be optionally substituted with halogen.
27. A process according to claim 26 wherein R3" in the coupling component represents methyl, ethyl or propyl substituted with chlorine.
28. A process according to claim 26 wherein there is used a coupling component of the formula wherein R1" has the same meaning as in claim 26.
29. A process according to claim 19 wherein there is used a coupling component of the formula
30. A process according to claim 19 wherein there is used a coupling component of the formula
31. A process according to claim 19 wherein there is used a coupling component of the formula
32. A process according to claim 19 wherein there is used a coupling component of the formula
33. A process according to claim 19 or 20 wherein there is used a coupling component of the formula
34. A process according to claim 19 or 20 wherein there is used a coupling component of the formula
35. A process according to claim 19 or 20 wherein there is used a coupling component of the formula
36. A process according to claim 19 or 20 wherein there is used a coupling component of the formula
37. A process of dyeing or printing, which comprises using an azo dye according to claim 1 for dyeing or printing synthetic fibres.
38. A process according to claim 37, for dyeing or printing fibres containing ester groups.
39. A process according to claim 37, for dyeing or printing polyester fibres.
40. The synthetic fibre material dyed and printed with the azo dyes according to claim 1.
CA299,037A 1977-03-16 1978-03-14 Azo dyes, processes for producing them, and their use Expired CA1109063A (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
LU76960 1977-03-16
LU76960A LU76960A1 (en) 1977-03-16 1977-03-16

Publications (1)

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CA1109063A true CA1109063A (en) 1981-09-15

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JP (1) JPS53113831A (en)
CA (1) CA1109063A (en)
CH (1) CH633306A5 (en)
DE (1) DE2811067C3 (en)
FR (1) FR2383994A1 (en)
GB (1) GB1600893A (en)
LU (1) LU76960A1 (en)

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6069276A (en) * 1999-03-05 2000-05-30 Milliken & Company Oxyalkylene-substituted m-amidoaniline intermediate

Family Cites Families (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
BE634032A (en) *
FR1361053A (en) * 1963-06-22 1964-05-15 Hoechst Ag Water insoluble monoazo dyes and their preparation
FR1534269A (en) * 1966-08-12 1968-07-26 Mitsui Kagaku Kogyo Kabushiki New monoazo dyes
GB1352059A (en) * 1970-05-06 1974-05-15 Sandoz Ltd Monoazo compounds of low solubility in water their production and use as dyes
GB1565531A (en) * 1976-02-05 1980-04-23 Ici Ltd Diperse monoazo dyestuffs

Also Published As

Publication number Publication date
CH633306A5 (en) 1982-11-30
DE2811067B2 (en) 1981-01-08
FR2383994A1 (en) 1978-10-13
LU76960A1 (en) 1978-10-18
DE2811067C3 (en) 1981-12-03
FR2383994B1 (en) 1980-06-13
GB1600893A (en) 1981-10-21
DE2811067A1 (en) 1978-09-21
JPS53113831A (en) 1978-10-04

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