Flame-resistant polycarbonate ABS moulding compounds

Details Flame-resistant polycarbonate ABS moulding compounds Flame-resistant polycarbonate ABS moulding compounds

2000-07-07

2004-02-03

Harlan, Robert (Department: 1713)

Synthetic resins or natural rubbers -- part of the class 520 ser

Synthetic resins

Processes of preparing a desired or intentional composition...

C524S141000, C524S240000, C524S375000, C524S430000, C524S444000

Reexamination Certificate

active

06686404

ABSTRACT:

The present invention relates to polycarbonate-ABS moulding compositions which exhibit excellent flane-resistance, and which contain, as a flame-retardant combination, oligomeric phosphorus compounds with an average degree of polycondensation of >5 and inorganilc nanoparticles and/or monophosphates.
EP-A 0 640 655 describes moulding compositions which comprise aromatic polycarbonates, copolymers which contain styrene, and graft polymers, and which can be made flame-retardant by treating them with monomeric and oligomeric phosphorus compounds with a degree of polycondensation of 1 to 2.
EP-A 0 363 608 describes flame-retardant polymer mixtures of aromatic polycarbonates, copolymers which contain styrene, or graft polymers, as well as oligomeric phosphates as flame-retardant additives. In order to achieve a satisfactory degree of flame-retardancy, the degree of polycondensation has to be within the range from 1.2 to 1.7. Examples verify that a degree of polycondensation of 2.8 results in unsatisfactory flame-retardancy.
EP-A 0 103 230 describes moulding compositions comprising special polycarbonates, copolymers which contain styrene, or graft polymers, and to which flame-resistance can likewise be imparted with polyphosphates. The polyphosphates which are used preferably have a degree of polycondensation from 4 to 25, wherein, in order to achieve flame-resistance, either a second halogen-containing flame-retardant has to be used in combination with the polyphosphates or the polyphosphates have to be used in relatively large amounts.
The object of the present invention was therefore to produce flame-retardant polycarbonate-ABS moulding compositions to which outstanding flame-retardancy can be imparted by treating them with phosphorus compounds, which have an average degree of polycondensation which is as high as possible, in conventional amounts in order to keep the tendency of the flame-retardant to migrate to the surface during processing as low as possible. The object was also that the polycarbonate-ABS moulding compositions should have good mechanical properties.
Surprisingly, this has been achieved by the use of oligomeric phosphorus compounds, preferably phosphate compounds, with a degree of polycondensation >5, in conventional amounts, in combination with inorganic nanoparticles and/or monophosphorus compounds.
The present invention therefore relates to flame-retardant thermoplastic moulding compositions containing
A. 5 to 95, preferably 30 to 90 parts by weight, particularly preferably 50 to 80 parts by weight, of an aromatic polycarbonate or polyestercarbonate,
B. 0.5 to 60, preferably 1 to 40 parts by weight, particularly preferably 2 to 25 parts by weight, of at least one graft polymer of
B.1 5 to 95, preferably 30 to 80 wt. % of one or more vinyl monomers on
B.2 95 to 5, preferably 70 to 30 wt. % of one or more graft substrates with a glass transition temperature <1.0° C., preferably <0° C., particularly preferably <−20° C.,
C. 0 to 45, preferably 0 to 30, particularly preferably 2 to 25 parts by weight of a thermoplastic vinyl copolymer,
D. 0.5 to 20 parts by weight, preferably 1 to 18 parts by weight, particularly preferably 2 to 15 parts by weight, of at least one phosphorus compound of general formula (I)
 wherein
R
1
, R
2
, R
3
, and R
4
, independently of each other, each represent C
1
- to C
8
-alkyl, C
5
- to C
6
-cycloalkyl, C
6
- to C
20
-aryl or C
7
- to C
12
-aralkyl, which are optionally halogenated,
n represents 0 or 1, which are independent of each other, and preferably represents 1,
N is a number from 5 to 30, preferably 5.5 to 20, particularly preferably 6 to 10,
wherein for mixtures of oligomeric phosphorus compounds the average degree of polycondensation N of component D is >5, and
X represents a mono- or polynuclear aromatic radical containing 6 to 30 carbon atoms, which is optionally substituted,
E 0 to 5 parts by weight, preferably 0.15 to 1 part by weight, particularly preferably 0.1 to 0.5 parts by weight of a fluorinated polyolefin, and
F.1 0.5 to 40, preferably 1 to 25, particularly preferably 2 to 15 parts by weight of a very finely divided inorganic powder with an average particle diameter of less than or equal to 200 nm, and/or
F.2 0.5 to 20, preferably 1 to 18, particularly preferably 2 to 15 parts by weight of a monophosphorus compound of formula (IA)
 wherein
R
11
, R
12
, and R
13
, independently of each other denote C
1
-C
5
-alkyl, which is optionally halogenated, or C
6
-C
20
-aryl, which is optionally halogenated,
ml denotes 0 or 1, and
nl denotes 0 or 1,
wherein the sum of all the parts by weight of A+B+C+D+E+F is 100.
Moulding compositions which are also quite particularly preferred are those in which the ratio by weight of components B:C, provided that C is present, is between 2:1 and 1:4 preferably between 1:1 and 1:3.
Component A
Aromatic polycarbonates and/or aromatic polyestercarbonates corresponding to component A which are suitable according to the invention are known from the literature or can be produced by methods which are known from the literature (for the production of aromatic polycarbonates, see Schnell, “Chemistry and Physics of Polycarbonates”, Interscience Publishers, 1964, as well as DE-AS 1 495 626, DE-OS 2 232 877, DE-OS 2 703 376, DE-OS 2 714 544, DE-OS 3 000 610 or DE-OS 3 832 396, for example; for the production of aromatic polyestercarbonates, see DE-OS 3 077 934 for example).
Aromatic polycarbonates are prepared, for example, by the reaction of diphenols with carbonic acid halides, preferably phosgene, and/or with aromatic dicarboxylic acid dilhalides, preferably benzenedicarboxylic acid dihalides, by the phase boundary process, optionally with the use of chain terminators, for example monophenols, and optionally with the use of trifunctional branching agents or branching agents with a functionality greater than three, for example triphenols or tetraphenols.
Diphenols for the production of aromatic polycarbonates and/or aromatic polyestercarbonates are preferably those of the formula (II)
wherein
A denotes a single bond, a C
1
-C
5
alkylene, C
2
-C
5
alkylidene, C
5
-C
6
cycloalkylidene, —O—, —SO—, —CO—, —S—, —SO
2
— a C
6
-C
12
-arylene radical, which can be condensed with other rings which optionally contain heteroatoms, a radical of formula (III)
or a radical of formula (IV)
radicals B, independent of each other, each denote a C
1
-C
8
alkyl radical, preferably methyl, a halogen, preferably chlorine and/or bromine, a C
6
-C
10
-aryl radical, preferably phenyl, or a C
7
-C
12
-aralkyl radical, preferably benzyl,
x denotes 0, 1 or 2, which are independent of each other in each case,
p is 1 or 0, and
R
5
and R
6
can be selected individually and independently of each other for each X
1
, and denote hydrogen or C
1
-C
6
-alkyl, preferably hydrogen, methyl or ethyl,
X
1
denotes carbon, and
m denotes an integer from 4 to 7, preferably 4 or 5, with the proviso that R
5
and R
6
simultaneously denote alkyl on at least one X
1
atom.
The preferred diphenols are hydroquinone, resorcinol, dihydroxydiphenols, bis-(hydroxyphenyl)-C
1
-C
5
-alkanes, bis-(hydroxyphenyl)-C
5
-C
6
-cycloalkanes, bis-(hydroxyphenyl) ethers, bis-(hydroxyphenyl) sulfoxides, bis-(hydroxyphenyl) ketones, bis-(hydroxyphenyl) sulfones and &agr;,&agr;-bis-(hydroxyphenyl)-diisopropyl-benzenes and ring-brominiated and/or ring-chlorinated derivatives thereof.
The diphenols which are particularly preferred are 4,4′-dihydroxydiphenyl, bisphenol A, 2,4-bis-(4-hydroxyphenyl)-2-methylbutane, 1,1-bis-(4-hydroxyphenyl)-cyclohexane, 1,1-bis-(4-hydroxyphenyl)-3,3,5-trimethylcyclohexane, 4,4′-dihydroxydiphenyl sulfide, 4,4′-dihydroxydiphenylsulfone, and di- and tetrabrominated or chlorinated derivatives thereof, such as 2,2-bis-(3-chloro-4-hydroxyphenyl)-propane, 2,2-bis-(3,5-dichloro-4-hydroxyphenyl)-propane or 2,2-bis-(3,5-dibromo-4-hydroxyphenyl)-propane for example.
2,2-bis-(4-hydroxyphenyl)-propane (bisphenol A) is particularly preferred.
The diphenols may be u

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