Flame-resistant reinforced polycarbonate ABS moulding materials

Details Flame-resistant reinforced polycarbonate ABS moulding materials Flame-resistant reinforced polycarbonate ABS moulding materials

2000-02-07

2002-08-27

Medley, Margarat (Department: 1714)

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

Synthetic resins

Processes of preparing a desired or intentional composition...

C525S067000, C525S462000

Reexamination Certificate

active

06441068

ABSTRACT:

The present invention relates to reinforced polycarbonate ABS moulding compositions flame-proofed with organic phosphorus compounds which have an excellent mechanical property level.
Reinforced flame-proofed polycarbonate ABS moulding compositions are already known.
Inter alia, EP-A-0 754 531 describes flame-proof moulding compositions consisting of polycarbonate, ABS graft polymer and optionally SAN copolymers which are reinforced with foliate inorganic materials.
Flame-proof polymer mixtures consisting of aromatic polycarbonate, styrene-containing copolymer and/or graft polymer, oligomeric phosphates as flame-proofing agents and fibres as reinforcing agents are known from EP-A-0 363 608.
The teaching of EP-A-0 640 655 relates to flame-proof moulding compositions consisting of aromatic polycarbonates, styrene-containing copolymers, graft polymers, and a mixture of mono- and oligomeric phosphates, which may optionally contain glass fibres as reinforcing materials.
For certain applications, such as for the production of moulded bodies with increased mechanical stress or for moulded bodies with thin wall thickness, the known moulding compositions exhibit an inadequate property level, particularly too little rigidity or insufficient flow behaviour.
The object of the present invention was therefore to provide flame-proof, reinforced polycarbonate ABS moulding compositions which have an excellent E modulus in addition to very good flame-proofness, very good processing properties and a high mechanical property level.
Surprisingly it has now been found that by the use of certain mixtures of polycarbonates, each with distinctly different solution viscosities, polycarbonate ABS moulding compositions result which have a distinctly better E modulus, higher notch impact strength and better processing behaviour than moulding compositions which contain as polycarbonate component only a polycarbonate with a corresponding average solution viscosity.
The invention therefore provides flame-proof, reinforced thermoplastic moulding compositions, containing
A. 5 to 95, preferably 10 to 90, particularly preferably 20 to 80 parts by weight of a mixture of two aromatic polycarbonates A.1 and A.2 with different solution viscosity, wherein
1. the relative solution viscosity of A.1 is 1.18 to 1.24,
2. the relative solution viscosity of A.2 is 1.24 to 1.34 and
3. the difference between the relative solution viscosities of A.1 and A.2 is not less than 0.06,
 wherein one or more further polycarbonates may be added to the mixture of A.1 and A.2,
B. 0 to 50, preferably 1 to 30, particularly preferably 2 to 25 parts by weight of a vinyl (co)polymer consisting of one or at least two ethylenically unsaturated monomers,
C. 0.5 to 60, preferably 1 to 40, particularly preferably 2 to 30 parts by weight of graft polymer with a glass transition temperature <−10° C. obtainable by graft polymerization of at least two of the monomers selected from chloroprene, butadiene, isoprene, styrene, acrylonitrile, ethylene, propylene, vinyl acetate and (meth)acrylic acid ester with 1 to 18 C atoms in the alcohol component,
D. 0.5 to 20 parts by weight, preferably 1 to 18 parts by weight, particularly preferably 2 to 15 parts by weight, of phosphorus compound of formula (I)
 in which
R
1
, R
2
, R
3
and R
4
independently of each other mean optionally halogenated C
1
-C
4
-alkyl, C
5
-C
6
-cycloalkyl, C
6
-C
20
-aryl or C
7
-C
12
-aralkyl, optionally substituted by halogen and/or C
1
-C
4
-alkyl in each case,
n independently of each other means 0 or 1,
N means 0 to 30 and
X means a mono- or polynuclear aromatic group with 6 to 30 C atoms,
E 0.05 to 5 parts by weight, preferably 0.1 to 1 part by weight, particularly preferably 0.1 to 0.5 parts by weight of fluorinated polyolefin and
F. 1 to 40, preferably 3 to 30, particularly preferably 5 to 20 parts by weight of inorganic, preferably fibrous reinforcing material.
The sum of all parts by weight A+B+C+D+E+F is 100.
Component A
Thermoplastic aromatic polycarbonates suitable according to the invention as Component A are those based on diphenols of formula (II)
in which
A means a single bond, C
1
-C
5
-alkylene, C
2
-C
5
-alkylidene, C
5
-C
6
-cycloalkylidene, —S—, —SO
2
—, —O—, —CO— or a C
6
-C
12
-arylene group which may optionally be condensed with further aromatic rings containing heteroatoms,
B independently of each other means in each case C
1
-C
8
-alkyl, preferably methyl, ethyl, C
6
-C
10
-aryl, preferably phenyl, C
7
-C
12
-aralkyl, preferably benzyl, halogen, preferably chlorine, bromine,
x independently of each other means 0, 1 or 2 in each case and
p means 1 or 0,
or alkyl-substituted dihydroxyphenyl cycloalkanes of formula (III)
in which
R
5
and R
6
independently of each other, in each case mean hydrogen, halogen, preferably chlorine or bromine, C
1
-C
8
-alkyl, preferably methyl, ethyl, C
5
-C
6
-cycloalkyl, C
6
-C
10
-aryl, preferably phenyl, and C
7
-C
12
-aralkyl, preferably phenyl-C
1
-C
4
-alkyl, particularly benzyl,
m means a whole number from 4 to 7, preferably 4 or 5,
R
7
and R
8
individually selectable for each Z and independently of each other mean hydrogen or C
1
-C
6
-alkyl, preferably hydrogen, methyl or ethyl, and
Z means carbon, with the proviso that R
7
and R
8
simultaneously mean alkyl on at least one atom Z.
Examples of suitable diphenols of formula (II) are hydroquinone, resorcinol, 4,4′-dihydroxydiphenyl, 2,2-bis-(4-hydroxyphenyl)-propane, 2,4-bis-(4-hydroxyphenyl)-2-methylbutane, 1,1-bis-(4-hydroxyphenyl)-cyclohexane, 2,2-bis-(3-chloro-4-hydroxyphenyl)-propane, 2,2-bis-(3,5-dibromo-4-hydroxyphenyl)-propane.
Preferred diphenols of formula (II) are 2,2-bis-(4-hydroxyphenyl)-propane, 2,2-bis-(3,5-dichloro-4-hydroxyphenyl)-propane and 1,1-bis-(4-hydroxyphenyl)-cyclohexane.
Preferred diphenols of formula (III) are dihydroxydiphenylcycloalkanes with 5 and 6 ring C atoms in the cycloaliphatic group [(m=4 or 5 in formula (III)] such as diphenols of the following formulae, for example:
wherein the 1,1-bis-(4-hydroxyphenyl)-3,3,5-trimethylcyclohexane (Formula IIIa) is particularly preferred.
The polycarbonates suitable according to the invention according to Component A may be branched in known manner, and indeed preferably by the incorporation of 0.05 to 2.0 mol %, related to the sum of the diphenols used, of tri- or more than trifunctional compounds, such as those with three or more than three phenolic groups, examples of which are:
phloroglucinol,
4,6-dimethyl-2,4,6-tri-(4-hydroxyphenyl)-heptene-2,
4,6-dimethyl-2,4,6-tri-(4-hydroxyphenyl)-heptane,
1,3,5-tri-(4-hydroxyphenyl)-benzene,
1,1,1-tri-(4-hydroxyphenyl)-ethane,
tri-(4-hydroxyphenyl)-phenylmethane,
2,2-bis-(4,4-bis-(4-hydroxyphenyl)-cyclohexyl)-propane,
2,4-bis-((4-hydroxyphenyl)-isopropyl)-phenol,
2,6-bis-(2-hydroxy-5′-methyl-benzyl)-4-methylphenol,
2-(4-hydroxyphenyl)-2-(2,4-dihydroxyphenyl)-propane,
hexa-(4-(4-hydroxyphenyl-isopropyl)-phenyl)-ortho-terephthalic acid ester,
tetra-(4-hydroxyphenyl)-methane,
tetra-(4-(4-hydroxyphenyl-isopropyl)-phenoxy)-methane and
1,4-bis-((4′,4″-dihydroxytriphenyl)-methyl)-benzene.
Some of the other trifunctional compounds are 2,4-dihydroxybenzoic acid, trimesic acid, cyanuric chloride and 3,3-bis-(3-methyl-4-hydroxyphenyl)-2-oxo-2,3-dihydroindole.
In addition to the bisphenol A homopolycarbonate, preferred polycarbonates are the copolycarbonates of bisphenol A with up to 15 mol %, related to the mol sum of diphenols, of 2,2-bis-(3,5-dibromo-4-hydroxyphenyl)-propane.
The aromatic polycarbonates of Component A may be partially replaced by aromatic polyester carbonates.
The aromatic polycarbonates of Component A may also contain polysiloxane blocks. Their manufacture is described, for example, in DE-OS 33 34 872 and U.S. Pat. No. 3,821,325.
Aromatic polycarbonates and/or aromatic polyester carbonates according to Component A are known in the literature or can be produced by processes known in the literature (on the production of aromatic polycarbonates see, for example,

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