Thermoplastic molding masses based on graft copolymers and...

Details Thermoplastic molding masses based on graft copolymers and... Thermoplastic molding masses based on graft copolymers and...

1997-06-18

2001-01-23

Niland, Patrick D. (Department: 1714)

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

Synthetic resins

Mixing of two or more solid polymers; mixing of solid...

C525S067000, C525S071000, C525S075000, C525S084000, C525S086000

Reexamination Certificate

active

06177517

ABSTRACT:

The present invention relates to thermoplastic molding compositions comprising
A) from 5 to 98% by weight, based on the total weight of the molding composition, of an elastomeric graft copolymer built up from
a
1
) from 30 to 90% by weight, based on A), of a graft base a
1
) built up from
a
11
) an at least partially crosslinked acrylate polymer formed from
a
111
) from 50 to 99.9% by weight, based on a
11
), of at least one C
1
-C
10
-alkyl acrylate,
a
112
) from 0.1 to 5% by weight, based on all), of a polyfunctional crosslinking monomer and
a
113
) from 0 to 49.9% by weight, based on all), of a further monomer which is copolymerizable with a
111
) selected from the group consisting of the vinyl C
1
C
8
-alkyl ethers, butadiene, isoprene, styrene, acrylonitrile and methacrylonitrile, and/or methyl methacrylate
and/or
a
12
) a diene polymer built up from
a
121
) from 50 to 100% by weight, based on a
12
), of a diene and
a
122
) from 0 to 50% by weight, based on a
12
), of other copolymerizable monomers selected from the group consisting of the vinyl C
1
-C
8
-alkyl ethers, C
1
-C
10
-alkyl acrylates, isoprene, styrene, acrylonitrile and methacrylonitrile, and/or methyl methacrylate,
and
a
2
) from 10 to 70% by weight, based on A), of a shell grafted onto the graft base, built up from
a
21
) from 50 to 95% by weight, based on a
2
), of a vinylaromatic monomer,
a
22
) from 5 to 50% by weight of polar, copolymerizable comonomers selected from the group consisting of acrylonitrile, methacrylo-nitrile, C
1
-C
4
-alkyl (meth)acrylates, maleic anhydride and maleimides, and (meth)acryl-amide, and/or vinyl C
1
-C
8
-alkyl ethers,
B) from 1 to 90% by weight, based on the total weight of the molding composition, of a copolymer made from
b
1
) from 50 to 99% by weight of a vinylaromatic monomer and
b
2
) from 1 to 50% by weight of monomers as described for a
22
),
C) from 1 to 70% by weight of an elastomeric block copolymer comprising at least one block CA which forms a hard phase and has in its polymer chain units of a vinylaromatic monomer
and/or of a block CB which forms a first elastomeric (soft) phase and comprises diene monomers
and at least one elastomeric block C
B/A
which forms a (if appropriate second or further) soft phase, and has in its polymer chain units of both a vinylaromatic monomer and a diene,
where the glass transition temperature T
g
of the block C
A
is above 25° C. and that of the block C
B/A
is below 25° C. and the phase-volume ratio of block C
A
to block C
B/A
is selected so that the proportion of the hard phase in the entire block copolymer is from 1 to 40% by volume, and the proportion by weight of the diene is less than 50% by weight,
D) from 0 to 300% by weight, based on the weight of components A) to C), of an aromatic polycarbonate,
E) from 0 to 20% by weight, based on the total weight of the molding composition, of conventional additives and processing aids.
Mixtures of thermoplastic polymers based on vinylaromatic polymers and graft elastomers are known to the person skilled in the art as ABS or ASA polymers, and are commercially available. Blends of such ASA and/or ABS polymers with other thermoplastics, in particular polycarbonates, are also known.
Owing to the introduction of ever faster processing machinery, such products of this type are expected to have, in particular, high flowability in injection molding and the ability to be demolded without breaking. In shaping by thermoforming, a high elongation at break is particularly important.
Various additives are generally used to optimize these properties, but these frequently improve only one parameter and in doing so impair another desired property. Thus additives for improving flowability and thermoforming properties frequently impair mechanical properties, whereas additives for improving demolding often impair flowability.
It is an object of the present invention, therefore, to provide thermoplastic molding compositions based on ABS polymers or ASA polymers which have a balanced property profile.
We have found that this object is achieved by means of the thermoplastic molding compositions as claimed in claim
1
.
Preferred embodiments of the invention are seen in the subclaims.
The novel molding compositions contain, as component A, from 5 to 98% by weight, preferably from 10 to 90% by weight, and in particular from 20 to 80% by weight, based on the total weight of the molding compositions, of an elastomeric graft copolymer.
This graft copolymer is built up from a graft base a
1
) with a glass transition temperature T
g
of below −10° C. and a graft a
2
) with a glass transition temperature T
g
of above 50° C., the proportion of the graft base a
1
) is from 30 to 90% by weight, preferably from 35 to 85% by weight, and in particular from 40 to 80% by weight, and that of the graft is correspondingly from 10 to 70% by weight, preferably from 15 to 65% by weight, and in particular from 20 to 60% by weight. The construction of the graft polymer A) is described in more detail below.
The graft base a
1
) is built up from
a
11
) an at least partially crosslinked acrylate polymer formed from
a
111
) from 50 to 99.9% by weight, based on all), of at least one C
1
-C
10
-alkyl acrylate,
a
112
) from 0.1 to 5% by weight, based on all), of a polyfunctional crosslinking monomer and
a
113
) from 0 to 49.9% by weight, based on all), of a further monomer which is copolymerizable with a
111
) selected from the group consisting of the vinyl C
1
-C
8
-alkyl ethers, butadiene, isoprene, styrene, acrylonitrile and methacrylonitrile, and/or methyl methacrylate
and/or
a
12
) a butadiene polymer built up from
a121) from 50 to 100% by weight, based on a
12
), of one or more dienes and
a
122
) from 0 to 50% by weight, based on a
12
), of further copolymerizable monomers selected from the group consisting of the vinyl C
1
-C
8
-alkyl ethers, C
1
-C
10
-alkyl acrylates, isoprene, styrene, acrylonitrile and methacrylonitrile, and/or methyl methacrylate.
Thus the molding compositions which can be used according to the invention comprise, in component A, either only one polymer a
11
) or a
12
) or a mixture of two polymers a
11
) and a
12
) as graft base.
When mixtures of polymers a
11
) and a
12
) are used, the mixing ratio is not critical, but is in general in the range from 4:1 to 1:4, in particular from 1:2 to 2:1.
The acrylate polymers all) are built up from
a
111
), from 50 to 99.9% by weight, preferably from 55 to 98% by weight, and in particular from 60 to 90% by weight, of a C
1
-C
10
-alkyl acrylate. C
2
-C
10
-alkyl acrylates are preferred, in particular ethyl acrylate, tert-, iso- and n-butyl acrylate and 2-ethylhexyl acrylate, the two last-mentioned being very particularly preferred.
Particular examples of crosslinking monomers a
112
) used in amounts of from 0.1 to 5% by weight, preferably from 0.25 to 4% by weight, and in particular from 0.5 to 3% by weight, based on all), are polyfunctional monomers having at least 2 non-conjugated olefinic double bonds, such as divinylbenzene, dialkyl fumarate, diallyl phthalate, triallyl cyanurate, trialkyl isocyanurate, tricyclodecenyl acrylate and dihydrodicyclopentadienyl acrylate. Tricyclodecenyl acrylate and dihydrodicyclopentadienyl acrylate are particularly preferred.
Other monomers a
113
) which may be used in the preparation of a
11
) are up to 49.9% by weight, preferably from 5 to 44.9% by weight, and in particular from 10 to 39.9% by weight of monomers which are copolymerizable with a
111
) selected from the group consisting of the vinyl C
1
-C
8
-alkyl ethers (eg. vinyl methyl ether, vinyl propyl ether, vinyl ethyl ether), butadiene, isoprene, styrene, acrylonitrile and methacrylonitrile and/or methacrylonitrile.
The use of comonomers of this type allows the property profile of the polymers all) to be controlled, eg. with respect to degree of crosslinking, which control can be desirable in many cases.
Processes for preparing polymers all) are known to the person skilled in the art and are described in the literature. Products of this type are also commerci

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