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
2001-03-28
2003-05-13
Cain, Edward J. (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...
C523S500000
Reexamination Certificate
active
06562902
ABSTRACT:
The invention relates to unreinforced thermoplastic molding compositions, moldings made therefrom, and also to the use of the molding compositions to produce the moldings.
Moldings made from polymeric materials and used in the interior of motor vehicles have to meet high requirements for heat resistance, mechanical properties, surface properties, aging performance, and also odor performance. Various polymeric materials are currently used to produce moldings for interior applications in motor vehicles.
One material used is ABS. This material has poor UV resistance, poor heat-aging resistance and poor heat resistance (Vicat B softening point<110° C.).
Another material used is ABS/PC (a polymer blend made from acrylonitrile-butadiene-stryene copolymer and polycarbonate). However, this material has unsatisfactory UV resistance, poor heat-aging performance (toughness and elongation at break after heat-aging), disadvantageous surface properties, poor stress cracking resistance for example with respect to plasticizers, and also in particular poor emission properties and poor odor performance. For the purposes of the present invention, odor performance is the tendency of materials, after a specified duration of aging under particular temperature and climatic conditions, to give off volatile constituents which have a discernible odor.
Another material used is ABS/PA (a polymer blend made from ABS and polyamide). ABS/PA, too, has poor UV resistance, poor heat resistance (Vicat B softening point<105° C.), poor heat-aging resistance, high moisture absorption, and also poor flowability.
Another material used is PPE/HIPS (a polymer blend made from polyphenylene oxide and impact-modified polystyrene). Disadvantages of this material are poor flowability, poor UV resistance, foam adhesion and heat-aging resistance, and also poor odor performance.
PET/PC (a polymer blend made from polyethylene terephthalate and polycarbonate) is also used. Disadvantages of this material are its low stress cracking resistance, for example with respect to plasticizers, and also its poor flowability.
PBT/PC is another material used. It has poor flowability and stress cracking resistance.
Most of the materials mentioned above have poor heat resistance, expressed in terms of a low Vicat B softening point (Vicat B<130° C.), and also poor heat-aging resistance. Good heat resistance and heat-aging resistance of the materials used is, however, essential since the temperature of the motor vehicle interior can rise considerably, especially when exposed to solar radiation.
The disadvantages mentioned above can be removed by using polymeric materials based on PBT/ASA/PSAN (polymer blends made from polybutylene terephthalate, acrylonitrile-styrene-acrylate copolymer and polystyrene-acrylonitrile copolymer). Materials of this type are generally disclosed in DE-A 39 11 828. The working examples relate to molding compositions in which the PSAN copolymers have a high proportion of acrylonitrile. However, like most of the abovementioned materials, moldings made from these molding compositions have poor emission performance and poor odor performance. The glass-fiber content of these molding compositions also has a disadvantageous effect on surface properties and on the toughness of moldings made from the compositions.
It is an object of the present invention to provide molding compositions suitable for producing moldings which are used in the interior of motor vehicles and have an advantageous property profile in terms of their mechanical, optical and surface properties, and also in particular have good heat resistance and heat-aging resistance, and good emission performance and/or odor performance.
We have found that this object is achieved by means of a thermoplastic molding composition comprising, based on the total of components A to C and, if desired, D and E, which in total give 100% by weight,
a) as component A, from 10 to 98% by weight of at least one aromatic polyester,
b) as component B, from 1 to 50% by weight of at least one particulate graft copolymer whose soft phase has a glass transition temperature below 0° C. and whose median particle size is from 50 to 1000 nm,
c) as component C, from 1 to 50% by weight of at least one copolymer made from the following monomers
c1) as component C1, from 50 to 90% by weight of at least one vinylaromatic monomer, and
c2) as component C2, from 10 to 25% by weight of acrylonitrile and/or methacrylonitrile,
d) as component D, from 0 to 25% by weight of other compatible polymers homogeneously miscible with components A and/or C or dispersible in these, and
e) as component E, from 0 to 10% by weight of conventional additives, such as UV stabilizers, carbon black, pigments, oxidation retarder, lubricants and mold-release agents.
The novel molding composition comprises, as component A, from 10 to 98% by weight, preferably from 20 to 75% by weight, particularly preferably from 30 to 60% by weight, of an aromatic polyester. The polyesters present in the novel molding compositions are known per se.
The polyesters may be prepared by reacting terephthalic acid, its esters or other ester-forming derivatives, with 1,4-butanediol, 1,3-propanediol or, respectively, 1,2-ethanediol, in a manner known per se.
Up to 20 mol % of the terephthalic acid may be replaced by other dicarboxylic acids. Those which may be mentioned, merely as examples, are naphthalenedi-carboxylic acids, isophthalic acid, adipic acid, azeleic acid, sebacic acid, dodecanedioic acid and cyclohexanedicarboxylic acids, mixtures of these carboxylic acids, and ester-forming derivatives of the same.
Up to 20 mol % of the dihydroxy compounds 1,4-butanediol, 1,3-propanediol or, respectively, 1,2-ethanediol may be replaced by other dihydroxy compounds, e.g. 1,6-hexanediol, 1,4-hexanediol, 1,4-cyclohexanediol, 1,4-di(hydroxymethyl)cyclohexane, bisphenol A, neopentyl glycol, mixtures of these diols, or also ester-forming derivatives of the same.
Preferred aromatic polyesters are polyethylene terephthalate (PET), polytrimethylene terephthalate (PTT) and in particular polybutylene terephthalate (PBT), whose formation involves exclusively terephthalic acid and the appropriate diols 1,2-ethanediol, 1,3-propanediol and 1,4-butanediol. Some or all of the aromatic polyesters may be used in the form of recycled polyester materials, such as PET regrind from bottle material or from wastes from bottle production.
In a particularly preferred embodiment component A is composed of
a1) from 60 to 100% by weight, in particular from 80 to 95% by weight, of polybutylene terephthalate, and
a2) from 0 to 40% by weight, in particular from 5 to 20% by weight, of polyethylene terephthalate.
The novel molding composition comprises, as component B, from 1 to 50% by weight, preferably from 1 to 25% by weight, particularly preferably from 2 to 15% by weight, in particular from 2 to 10% by weight, of at least one particulate graft copolymer with a glass transition temperature of the soft phase below 0° C. and with a median particle size of from 50 to 1000 nm.
Component B is preferably a graft copolymer made from
b1) from 50 to 90% by weight of a particulate graft base B1 with a glass transition temperature below 0° C., and
b2) from 10 to 50% by weight of a graft B2 made from the following monomers
b21) as component B21, from 50 to 90% by weight of a vinylaromatic monomer, and
b22) as component B22, from 10 to 49% by weight of acrylonitrile and/or methacrylonitrile.
The particulate graft base B1 may be composed of from 70 to 100% by weight of a conjugated diene and from 0 to 30% by weight of a bifunctional monomer having two non-conjugated olefinic double bonds. Graft bases of this type are used, for example, as component B in ABS polymers or MBS polymers.
In a preferred embodiment of the invention the graft base B1 is composed of the following monomers:
b11) as component B11, from 75 to 99.9% by weight of a C
1
-C
10
-alkyl acrylate,
b12) as component B12, from 0.1 to 10% by weight of at least one polyfunctional monomer having at least two non-conjugated o
Berz Stephan
Fischer Michael
Ginss Christophe
Knoll Manfred
BASF - Aktiengesellschaft
Cain Edward J.
Keil & Weinkauf
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