Flame resistant ABS polycarbonate mouldable materials

Details Flame resistant ABS polycarbonate mouldable materials Flame resistant ABS polycarbonate mouldable materials

2000-02-07

2004-06-22

Szekely, Peter (Department: 1714)

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

Synthetic resins

Processes of preparing a desired or intentional composition...

C524S145000

Reexamination Certificate

active

06753366

ABSTRACT:

The present invention relates to polycarbonate-ABS moulding compositions which are made flame-retardant with phosphorus compounds, and which exhibit an excellent level of mechanical properties, particularly a considerably improved ultimate tensile strength and yield stress as well as an outstanding tensile modulus of elasticity.
EP-A-0 363 608 describes polymer mixtures comprising an aromatic polycarbonate and a copolymer or graft copolymer containing styrene, as well as oligomeric phosphates as flame retardant additives. The level of mechanical properties of these mixtures is often unsatisfactory for certain purposes of use.
EP-A-0 704 488 describes moulding compositions comprising an aromatic polycarbonate, copolymers which contain styrene, and graft polymers with a special graft base, in defined quantitative ratios. These moulding compositions have a very good notched bar impact strength, and can optionally be made flame-retardant with phosphorus compounds. Their level of mechanical properties is not always satisfactory for the production of mouldings which are subject to intensified elastic loading.
The object of the present invention is therefore to provide flame-retardant polycarbonate-ABS moulding compositions which, in addition to the requisite high level of flame-retardancy, have an excellent ultimate tensile strength and an excellent tensile modulus of elasticity.
It has now been found that PC/ABS moulding compositions, which contain phosphorus compounds according to component D (see below) and a graft polymer comprising a graft base of defined particle size, can be processed to form mouldings with a very good level of mechanical properties, particularly under intensified elastic loading also.
The present invention therefore relates to a flame-retardant thermoplastic moulding composition containing
A. 40 to 99, preferably 60 to 98.5 parts by weight, of an aromatic polycarbonate or polyester carbonate
B. 0.5 to 60, preferably 1 to 40, particularly 2 to 25 parts by weight, of a graft polymer of
B.1 5 to 95, preferably 30 to 80% by weight, of one or more vinyl monomers on
B.2 95 to 5, preferably 20 to 70% by weight of one or more graft bases with a glass transition temperature <0° C., preferably <−20° C., and an average particle size (d
50
value) of 0.20 to 0.35 &mgr;m, preferably 0.25 to 0.30 &mgr;m
C. 0 to 45, preferably 0 to 30, most preferably 2 to 25 parts by weight of a thermoplastic vinyl (co)polymer
D. 0.5 to 20 parts by weight, preferably 1 to 18 parts by weight, most preferably 2 to 15 parts by weight, of at least one mono- and at least one oligophosphorus compound of general formula (I)
wherein
R
1
, R
2
, R
3
and R
4
, independently of each other, each denote a C
1
to C
8
alkyl which is optionally halogenated in each case, a C
5
to C
6
cycloalkyl, C
6
to C
20
aryl or C
7
to C
20
aralkyl, which are each optionally substituted by an alkyl, preferably a C
1
-C
4
alkyl and/or by a halogen, preferably chlorine or bromine,
n denotes 0 or 1, which are independent of each other.
N denotes 0 to 30, and
X denotes a mono- or polynuclear aromatic radical containing 6 to 30 C atoms; and
E. denotes 0.05 to 5 parts by weight, preferably 0.1 to 1 parts by weight, most preferably 0.1 to 0.5 parts by weight, of a fluorinated polyolefine,
wherein the sum of all the parts by weight of A+B+C+D+E is 100.
Moulding compositions which are particularly preferred are those in which the ratio by weight of components B:C is between 2:1 and 1:4, preferably between 1:1 and 1:3.
In the moulding compositions according to the invention, component D is preferably present as a mixture of 10 to 90% by weight, preferably 12 to 40% by weight, of at least one monophosphorus compound of formula (I), and 10 to 90% by weight, preferably 60 to 88% by weight, with respect to the total amount of phosphorus compounds in each case, of at least one oligophosphorus compound of formula (I), wherein the mixture has an average N of 0.3 to 20, preferably 0.5 to 10, most preferably 0.5 to 6.
COMPONENT A
Aromatic polycarbonates and/or aromatic polyester carbonates according to component A which are suitable according to the invention are known from the literature or can be produced by methods known from the literature (for example, 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 and DE-OS 3 832 396; for the production of aromatic polyester carbonates see DE-OS 3 077 934 for example).
The production of aromatic polycarbonates is effected, for example, by the reaction of diphenols with carbonic acid halides, preferably phosgene, and/or with aromatic dicarboxylic acid dihalides, preferably benzenedicarboxylic acid dihalides, by the phase boundary method, optionally with the use of chain terminators e.g. monophenols, and optionally with the use of trifunctional branching agents or branching agents with a functionality higher than three, for example triphenols or tetraphenols.
Diphenols for the production of the aromatic polycarbonates and/or aromatic polyester carbonates are preferably those of formula (II)
wherein
A denotes a single bond, a C
1
-C
5
alkylene, a C
2
-C
5
alkylidene, a C
5
-C
6
cycloalkylidene, —O—, —SO—, —CO—, —S—, —SO
2
—, or a C
6
-C
12
arylene, on to which other aromatic rings, which optionally contain hetero atoms, can be condensed,
or a radical of formula (III) or (IV)
B denotes hydrogen a C
1
-C
12
alkyl, preferably methyl, or a halogen, preferably chlorine and/or bromine, in each case
x is 0.1 or 2, independently of each other, in each case.
p is 1 or 0, and
R
5
and R
6
, which are independent of each other and are individually selectable for each X
1
, denote hydrogen or a 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 an 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)-sulphoxides, bis-(hydroxyphenyl)ketones, bis-(hydroxyphenyl)-sulphones and &agr;,&agr;′-bis-(hydroxyphenyl)-diisopropylbenzenes, as well as derivatives thereof which have brominated and/or chlorinated nuclei.
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 sulphide and 4,4,-dihydroxydiphenyl-sulphone, as well as 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.
2,2-bis-(4-hydroxyphenyl)-propane (bisphenol A) is particularly preferred.
The diphenols can be used individually or as arbitrary mixtures.
The diphenols are known from the literature or can be obtained by methods known from the literature.
Examples of suitable chain terminators for the production of the thermoplastic, aromatic polycarbonates include phenol, p-chlorophenol, p-tert.-butylphenol or 2,4,6-tribromophenol, as well as long chain alkylphenols such as 4-(1,3-tetramethyl-butyl)-phenol according to DE-OS 2 842 005 or monoalkylphenols or dialkylphenols which contain a total of 8 to 20 C atoms in their alkyl substituents, such as 3,5-di-tert.-butyl-phenol, p-iso-octylphenol, p-tert.-octylphenol, p-dodecylphenol, 2-(3,5-dimethylheptyl)-phenol and 4-(3,5-dimethylheptyl)-phenol. The amount of chain terminators used is generally between 0.5 mole % and 10 mole % with respect to the molar sum of the diphenols used in each case.
The thermoplastic, aromatic polycarbonates have mean weight average molecular weights (M
w
, as measured by ultracentrifuging or by sca

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