Molding compositions comprising random copolyamides, their...

Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – At least one aryl ring which is part of a fused or bridged...

Reexamination Certificate

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C524S504000, C524S508000, C524S511000, C524S514000, C525S066000, C525S09200D, C525S133000

Reexamination Certificate

active

06284830

ABSTRACT:

The invention relates to molding compositions comprising random copolyamides, a process for their preparation, their use for producing moldings, fibers or films, and moldings, fibers or films produced therefrom.
A wide variety of polyamide molding compositions, in particular in the form of polymer blends, is known, and in these the formulation of the molding compositions is matched to their desired property spectrum. In the case of glass-fiber-reinforced polyamide molding compositions in particular, it should be possible, besides advantageous mechanical properties, also to achieve a lustrous and smooth surface of the moldings produced therefrom. This should not impair the processing properties of the molding compositions, but in the case of glass-fiber-reinforced injection-molded materials, the surface of the moldings is frequently matt and rough because of unevenness, irregularities and the effect known as glass-fiber effect, and this is generally undesirable in visible moldings, which often influence the design of an article.
DE-C-43 21 247 describes polyamide resin compositions which, besides hexamethylene adipamide units made from adipic acid and hexamethylenediamine, also contain from 10 to 25% by weight of a hexamethylene isophthalamide made from isophthalic acid and hexamethylenediamine. The resin compositions also contain from 5 to 70% by weight of at least one inorganic filler, in particular glass fibers. The molding compositions are claimed to be homogeneous and to have good forming properties and high surface gloss, coupled with high strength, stiffness and dimensional stability. High surface gloss was a particular aim in these molding compositions.
JP-A 80/062 958 describes mixtures of polyamides and from 5 to 50% by weight of inorganic fibrous reinforcing materials. The polyamides here may have from 30 to 100% by weight of hexamethylene isophthalamide units. Hexamethylene isophthalamide polymers, hexamethylene isophthalamide-hexamethylene terephthalamide copolymers and hexamethylene isophthalamide-caproamide copolymers are in particular described.
JP-A 93/339 494 describes resin formulations having high strength and stiffness, low water absorption and good appearance. They comprise, for example, 20% by weight of a semiaromatic polyamide resin made from 50% by weight of hexamethylene adipamide units made from adipic acid and hexamethylenediamine, 30% by weight of hexamethylene isophthalamide units made from isophthalic acid and hexamethylenediamine and 20% by weight of hexamethylene terephthalamide units made from terephthalic acid and hexamethylenediamine, besides 80% by weight of a polyphenylene ether resin.
J. S. Ridgway, in J. Polym. Sc. Vol. 8, Part A-1, (1970), pages 3089 to 3111 describes structure-property relationships of nylon-6,6 copolyamides which contain ring structures. The ring structure was correlated here with the glass transition temperature and the melting point. Copolyamides are described which are based on adipic acid and hexamethylenediamine and contain from 10 to 30 mol % of isophthalic acid units.
WO 91/13194 describes improved starting materials for producing nylon yarns, for example random copolymers made from 87% by weight of adipic acid/hexamethylenediamine and 13% by weight of isophthalic acid/hexamethylenediamine, or 92% by weight of adipic acid/hexamethylenediamine and 8% by weight of isophthalic acid/hexamethylenediamine. From these, it is possible to obtain good yarns for carpet production.
EP-A-0 654 505 discloses high-molecular-weight thermoplastic molding compositions which are obtainable by incorporating a polyphenylene ether, is besides other additives and processing aids, into a melt of a low-molecular-weight polyamide, followed by post-condensation in the solid phase. The polyamides used were nylon-6,6 having a viscosity number in the range from 60 to 283 and a nylon-6/6,T having a viscosity number of 125.
EP-A-0 678 555 relates to thermoplastic molding compositions which comprise a partly aromatic, partially crystalline copolyamide and a polyphenylene ether. The copolyamide is built up from 30 to 44 mol % of terephthalic acid, from 6 to 20 mol % of isophthalic acid, from 43 to 49.5 mol % of hexamethylenediamine and from 0.5 to 7 mol % of aliphatic cyclic diamines.
EP-A-0 694 583 relates to thermoplastic molding compositions made from a partially crystalline, partly aromatic polyamide, polyolefin homo- or copolymers and compatibilizers. The copolyamide is built up from 30 to 44 mol % of terephthalic acid, from 6 to 20 mol % of isophthalic acid, from 43 to 49 mol % of hexamethylenediamine and from 0.5 to 7 mol % of aliphatic cyclic diamines.
EP-A-0 722 986 relates to thermoplastic molding compositions made from a partly aromatic, partially crystalline copolyamide, ASA or ABS or SAN polymers or C
1
-C
18
-alkyl (meth)acrylates and a compatibilizer. The copolyamide itself is built up from 30 to 44 mol % of terephthalic acid, from 6 to 20 mol % of isophthalic acid, from 43 to 49.5 mol % of hexamethylenediamine and from 0.5 to 7 mol % of aliphatic cyclic diamines.
DE-A-2 122 735 relates to a thermoplastic polymer mixture of an aromatic polysulfone and a polyamide. It is stated that the mixtures have desirable combinations of physical properties, although mixtures of different polymeric substances are usually mechanically weak.
EP-A-0 477 757 relates to polymer blends of polyaryl ether sulfones and polyamides, the polyamides having at least 50% by weight of recurring units of 1,6-hexamethylene terephthalamide. Besides good thermal properties and compatibility of the individual phases, the blends are claimed also to have a desirable combination of mechanical properties.
DE-A-41 21 705 relates to thermoplastic molding compositions based on polyarylene ethers and partly aromatic copolyamides. It is stated that mixtures of this type have excellent stiffness and high heat resistance.
DE-A-44 29 107 relates to molding compositions made from polyarylene ethers and copolyamides which have been built up from terephthalic acid, isophthalic acid, hexamethylenediamine and aliphatic cyclic diamines.
Besides high stiffness and heat resistance, the molding compositions are claimed to have good stability during processing.
The known molding compositions, in particular polyamide blends, do not have surface properties adequate for all applications, combined with good mechanical properties.
It is an object of the present invention to provide molding compositions comprising copolyamides, in particular copolyamide blends, which, besides very good mechanical properties, have very good surface quality and avoid the disadvantages of the known molding compositions. In particular, they should have high elongation at break and high modulus of elasticity. Their mechanical properties should be retained even after exposure to heat.
We have found that this object is achieved by providing a molding composition comprising components A, B and, if desired, components C to E, the total weight of which is 100% by weight:
a: as component A, from 5 to 95% by weight of a random copolyamide made from
a1: from 95.1 to 99.9% by weight of component A1 made from equimolar amounts of at least one linear aliphatic diamine and at least one linear aliphatic dicarboxylic acid
a2: from 0.1 to 4.9% by weight of component A2 made from equimolar amounts of at least one linear aliphatic diamine and isophthalic acid
b: from 5 to 95% by weight of a copolymer component B, different from component A, selected from:
b1: component B1 made from at least one, if desired modified, polyphenylene ether, or
b2: component B2 made from, as component B21, from 60 to 99% by weight of at least one polyolefm homo- or copolymer and, as component B22, from 1 to 40% by weight of at least one modified polyolefin homo- or copolymer, or
b3: component B3 made from, as component B31, from 70 to 100% by weight of at least one SAN, ABS or ASA polymer and, as component B32, from 0 to 30% by weight of at least one modified SAN, ABS or ASA polymer
c: as component C, from 0 to 20% by weight of at least one impact mo

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