Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Mixing of two or more solid polymers; mixing of solid...
Reexamination Certificate
2000-10-03
2003-02-11
Mullis, Jeffrey (Department: 1711)
Synthetic resins or natural rubbers -- part of the class 520 ser
Synthetic resins
Mixing of two or more solid polymers; mixing of solid...
C525S071000, C525S085000, C525S086000, C525S087000
Reexamination Certificate
active
06518361
ABSTRACT:
The present invention relates to thermoplastic molding compositions made from
A) from 20 to 98% by weight of a particulate graft polymer made from
a1) from 30 to 90% by weight of an elastomeric graft core made from
a11) from 80 to 99.99% by weight of a C
1
-C
10
-alkyl acrylate,
a12) from 0.01 to 20% by weight of at least one crosslinking monomer, and
a13) from 0 to 19.99% by weight of one or more other monomers,
a2) from 10 to 70% by weight of a graft shell made from
a21) from 50 to 100% by weight of a styrene compound of the formula I
where R
1
and R
2
are hydrogen or C
1
-C
8
-alkyl and n is 0, 1, 2 or 3,
a22) from 0 to 50% by weight of at least one monoethylenically unsaturated nitrile compound, and
a23) from 0 to 40% by weight of one or more other monomers,
B) from 0.5 to 78.5% by weight of a thermoplastic polymer made from
b1) from 50 to 100% by weight of a styrene compound of the formula
where R
1
and R
2
are hydrogen or C
1
-C
8
-alkyl and n is 0, 1, 2 or 3,
b2) from 0 to 50% by weight of at least one monoethylenically unsaturated nitrile compound, and
b3) from 0 to 40% by weight of one or more other monomers,
C) from 1 to 79% by weight of a copolymer made from
c1) from 30 to 90% by weight of styrene and/or &agr;-methylstyrene,
c2) from 10 to 70% by weight of butadiene, and
c3) from 0 to 30% by weight of one or more other monomers
in which all, or virtually all, of the olefinic double bonds have been hydrogenated, and
D) from 0.5 to 30% by weight of a copolymer made from
d1) from 50 to 100% by weight of isobutene, and
d2) from 0 to 50% by weight of one or more other monomers.
The invention further relates to the use of these molding compositions for producing films and moldings, and also to films and moldings made from these molding compositions and to a process for preparing the molding compositions.
The total of components A) to D) is, of course, 100% by weight.
There are many application sectors for plastic films. They are mostly produced by calendering or extrusion.
EP-A 526 813 has disclosed thermoplastic molding compositions made from a highly crosslinked acrylate rubber with a graft shell made from methyl methacrylate or styrene/acrylonitrile and with a partially crosslinked acrylate rubber and with an ethylene/vinyl acetate copolymer, and also if desired with another polymer based on styrene and/or acrylic compounds. Under the conditions of molding, for example to give films, these compositions tend, however, to give undesirable discoloration.
DE-A 42 11 412 has proposed, as a film material, mixtures of styrene/acrylonitrile polymers and thermoplastics, which have a graft shell made from an elastomeric polymer. However, the process for preparing graft polymers of this type is complicated and it is therefore difficult to obtain consistent product quality.
EP-A 708 145 has disclosed thermoplastic molding compositions which comprise an acrylate rubber with a graft shell made from styrene-acrylonitrile, and comprise a hard styrene-acrylonitrile matrix and a hydrogenated copolymer made from styrene and butadiene. The films obtainable therefrom are very tough and tear-resistant. However, the flowability of the molding compositions is not always adequate for extrusion processing, and therefore the reliability of the extrusion process, and also the quality of the extruded film product, are not fully satisfactory.
EP-A 693 530 teaches improvement of the impact strength of mixtures made from polycarbonate and diene graft rubbers or alkyl acrylate graft rubbers, by using functionalized polyisobutylene polymers. In DE-A 20 20 478 polyisobutene (PIB), also termed polyisobutylene, is used concomitantly in blends made from thermoplastics to improve the dielectric properties of the molding composition.
In an Amoco company publication “Amoco Polybutene” which appeared in 1994 it is reported on page 18 that polybutene improves the impact strength and elasticity of a wide variety of thermoplastics. The Amoco company publication of June 1995 “Acrylonitrile-Butadiene-Styrene Modification using Amoco Polybutene” discloses on page 5 that polybutene improves the impact strength of ABS (acrylonitrile-butadiene-styrene).
It is not disclosed in any of the publications mentioned that polybutene considerably improves the flowability and therefore the extrusion performance of films made from ASA (acrylonitrile-styrene-acrylate).
It is an object of the present invention to overcome the disadvantages described at the outset. A particular object is to provide molding compositions which have good flowability and good extrusion properties and can be extruded with high reliability of the process to give films or moldings of consistent product quality, and also having good and well balanced mechanical properties.
We have found that this object is achieved by means of the thermoplastic molding compositions defined at the outset.
The invention provides, furthermore, the use of the polymer mixture for producing films and moldings, and also films and moldings made from these compositions.
Component A) is present in the novel molding compositions in a proportion of from 20 to 98% by weight, preferably from 40 to 90% by weight and particularly preferably from 50 to 82% by weight, based on the total of components A) to D). This component is a particulate graft copolymer which has been built up from an elastomeric graft core al) (soft component) and, grafted onto this, a shell a2) (hard component).
The graft core a1) is present in a proportion of from 30 to 90% by weight, preferably from 40 to 80% by weight and in particular from 50 to 75% by weight, based on component A).
The graft core a1) is obtained by polymerizing a monomer mixture made from, based on a1),
a11) from 80 to 99.99% by weight, preferably from 85 to 99.5% by weight and particularly preferably from 90 to 99% by weight, of a C
1
-C
10
-alkyl acrylate,
a12) from 0.01 to 20% by weight, preferably from 0.5 to 10% by weight and particularly preferably from 1 to 5% by weight, of at least one crosslinking monomer, and
a13) from 0 to 19.99% by weight, preferably from 0 to 5% by weight, of one or more other monomers.
Particularly suitable alkyl acrylates a11) are ethyl acrylate, 2-ethylhexyl acrylate and especially n-butyl acrylate.
Crosslinking monomers a12) are bi- or polyfunctional comonomers, such as butadiene and isoprene, divinyl esters of dicarboxylic acids, such as succinic acid or adipic acid, diallyl or divinyl ethers of dihydric alcohols, such as of ethylene glycol or of 1,4-butanediol, diesters of acrylic acid and methacrylic acid with the dihydric alcohols mentioned, 1,4-divinylbenzene or triallyl cyanurate. Particular preference is given to the acrylate of tricyclodecenyl alcohol, known as dihydrodicyclopentadienyl acrylate, and also to the allyl esters of acrylic and methacrylic acids.
Replacing some of the monomers a11) and a12) in the graft core a1) of the molding compositions there may also be other monomers a13) which vary the mechanical and thermal properties of the core within a certain range. Examples which may be mentioned of such monoethylenically unsaturated comonomers are:
vinylaromatic monomers, such as styrene or styrene derivatives of the formula I
where R
1
and R
2
are hydrogen or C
1
-C
8
-alkyl and n is 0, 1, 2 or 3;
acrylonitrile, methacrylonitrile;
acrylic acid, methacrylic acid, dicarboxylic acids, such as maleic and fumaric acids, and also the anhydrides of these, such as maleic anhydride;
nitrogen-functional monomers, such as dimethylaminoethyl acrylate, diethylaminoethyl acrylate, vinylimidazole, vinylpyrrolidone, vinylcaprolactam, vinylcarbazole, vinylaniline and acrylamide;
C
1
-C
4
-alkyl methacrylates, such as methyl methacrylate, ethyl methacrylate, n-propyl methacrylate, isopropyl methacrylate, n-butyl methacrylate, isobutyl methacrylate, sec-butyl methacrylate, tert-butyl methacrylaue and hydroxyethylmethacrylate;
aromatic and araliphatic esters of acrylic or methacrylic acid, such as phenyl acrylate, phenyl methacrylate, benzyl acrylate, benzyl methacrylate, 2-phenylethyl acr
Güntherberg Norbert
Lindenschmidt Gerhard
Rath Hans Peter
Weber Martin
BASF - Aktiengesellschaft
Keil & Weinkauf
Mullis Jeffrey
LandOfFree
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