Moulding materials with a polyarylene ether sulfone and...

Details Moulding materials with a polyarylene ether sulfone and... Moulding materials with a polyarylene ether sulfone and...

2001-02-26

2003-01-21

Szekely, Peter (Department: 1714)

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...

C524S606000, C524S609000

Reexamination Certificate

active

06509403

ABSTRACT:

The present invention relates to molding compositions which comprise
A) at least one polyarylene ether sulfone,
B) at least one aliphatic polyamide,
C) at least one filler, and also if desired
D) an impact-modifying rubber or a mixture of various impact-modifying rubbers, and
E) an additive or a mixture of various additives, wherein the viscosity number of the polyamides B (measured in 0.5% strength by weight solution in 96% strength by weight sulfuric acid to DIN 53 727) is at least 180 ml/g, and the molding compositions also comprise
F) from 100 ppm to 0.5% by weight, based on the total weight of A to E, of a copper halide.
The present invention further relates to a process for preparing the molding compositions, and also to the use of these for producing moldings, and to the resulting moldings.
Molding compositions based on polyarylene ether sulfones with polyamides have been known for a long time.
For example, DE-A 41 21 705 and 44 29 107 have disclosed mixtures which comprise partially aromatic copolyamides alongside polyarylene ethers. The first of these publications discloses blends comprising preferably partially aromatic copolyamides with relative viscosities of from 2.2 to 5.0, implying viscosity numbers of from 120 to 400 ml/g. The copolyamides described in DE-A 44 29 107 preferably have viscosity numbers of from 100 to 500 ml/g, in particular from 110 to 200 ml/g. Blends made from polyarylene ether sulfones with polyamides and having at least 50% by weight of hexamethylene terephthalamide units have been disclosed in EP-A 477 757. Preference is given to blends made from these polyamides and having viscosity numbers of up to 140 ml/g (implying that &eegr;
red
is 1.4 dl/g), since the polyamides with higher viscosities (up to an &eegr;
red
of 1.9 dl/g) are difficult to process. The molding compositions described in the publications mentioned have good heat resistance, but if moldings made from them are heated above 150° C. for prolonged periods their mechanical properties become impaired. EP-A 513 488 describes molding compositions based on polyarylene ethers with polyamides and having improved adhesive strength and improved compatibility with fillers and with other thermoplastics, and suitable for producing thermally stable adhesives. The polyamides preferably used include aliphatic polyamides, such as nylon-6. The viscosities of the polyamides which can be used are from 120 to 400 ml/g (implying that &eegr;
rel
is from 2.0 to 5.0). The heat resistance of these mixtures is still inadequate for some applications.
It is an object of the present invention to improve the heat resistance of molding compositions based on polyarylene ethers with polyamides. In particular, the moldings obtainable from these should withstand long-term exposure to temperatures above 150° C. without significant impairment of their mechanical properties. The molding compositions should also be very easy to process, and they should in particular have good flowability. Another requirement placed upon the molding compositions was that they should be simple and cost-effective to produce.
We have found that this object is achieved by means of the molding compositions defined at the outset, which are described in more detail below.
Component A
The proportion of component A in the novel molding compositions can vary widely. Preferred molding compositions according to the invention comprise amounts of from 2 to 97.8% by weight, in particular from 5 to 94.8% by weight, of component A, based on the total weight of A to E. Particularly preferred molding compositions comprise from 7.5 to 92.3% by weight of component A, based on the total weight of A to E.
According to the invention component A is a polyarylene ether sulfone. Component A may also be a mixture made from two or more different polyarylene ether sulfones.
The arylene groups of the polyarylene ether sulfones A may be identical or different and, independently of one another, are an aromatic radical having from 6 to 18 carbon atoms. Examples of suitable arylene radicals are phenylene, biphenylene, terphenylene, 1,5-naphthylene, 1,6-naphthylene, 1,5-anthrylene, 9,10-anthrylene and 2,6-anthrylene. Among these, preference is given to 1,4-phenylene and 4,4′-biphenylene. These aromatic radicals are preferably unsubstituted. However, they may have one or more substituents. Examples of suitable substituents are alkyl, arylalkyl, aryl, nitro, cyano and alkoxy groups, and also heteroaromatics, such as pyridine, and halogen. Preferred substituents include alkyl having up to 10 carbon atoms, such as methyl, ethyl, isopropyl, n-hexyl and isohexyl, C
1
-C
10
-alkoxy radicals, such as methoxy, ethoxy, n-propoxy and n-butoxy, aryl radicals having up to 20 carbon atoms, such as phenyl and naphthyl, and also fluorine and chlorine. Other preferred substituents are those obtainable by reacting the polyarylene ether sulfones with a reactive compound which has, besides a carbon-carbon double or triple bond, one or more carbonyl, carboxylic acid, carboxylate, anhydride, amide, imide, carboxylic ester, amino, hydroxyl, epoxy, oxazoline, urethane, urea, lactam or halobenzyl groups. The bonding of the arylene groups to one another in the polyarylene ether may be via —SO
2
—, or, for example, via —O—, —S—, —SO—, —CO—, —N═N—, —COO—, or via an unsubstituted or substituted alkylene radical, or via a chemical bond.
Preferred polyarylene ether sulfones which can be used according to the invention (component A) have a structure made from recurring units of the formula I
where
x is 0.5 or 1,
t and q, independently of one another, are 0, 1, 2 or 3,
n is an integer from 0 to 6,
each of Q, T and Z, independently of one another, is a chemical bond or a group selected from the class consisting of —O—, —S—, —SO
2
—, S═O, C═O, —N═N , —R
a
C═CR
b
— and —CR
c
R
d
—,
where each of R
a
and R
b
, independently of one another, is hydrogen or C
1
-C
12
-alkyl and each of R
c
and R
d
, independently of one another, is hydrogen or C
1
-C
12
-alkyl, C
1
-C
12
-alkoxy or C
6
-C
18
-aryl, where, if desired, R
c
and R
d
may independently of one another have fluorine and/or chlorine substituents or, together with the carbon atom to which they are bonded, may form a C
3
-C
12
-cycloalkyl group, which may be unsubstituted or substituted by one or more C
1
-C
6
-alkyl groups, with the proviso that at least one of the groups T, Q and Z is —SO
2
— and if t and q are 0, Z is —SO
2
—, and
Ar, Ar
1
, Ar
2
and Ar
3
, independently of one another, are C
6
-C
18
-arylene, unsubstituted or substituted by C
1
-C
12
-alkyl, C
6
-C
18
-aryl, C
1
-C
12
-alkoxy or halogen.
Polyarylene ethers A which can be used according to the invention may be prepared, for example, in a manner similar to that of GB 1 152 035 and U.S. Pat. No. 4,870,153, which are expressly incorporated herein by way of reference. Examples of suitable process conditions for the synthesis of polyarylene ether sulfones are described in EP-A-0 113 112 and EP-A-0 135 130. The reaction of the monomers in aprotic polar solvents in the presence of anhydrous alkali metal carbonate is particularly suitable. A particularly preferred combination is N-methylpyrrolidone as solvent and potassium carbonate as catalyst. The reaction in the melt is similarly preferred. However, the introduction of terminal anhydride groups described there is not an essential requirement for the present invention. Examples of suitable polyarylene ether sulfones A are those having at least one of the following recurring structural units I
1
to I
15
: for x=0.5 in formula I:
Particularly preferred units of the formula I are those of the formulae I
1
and I
2
, individually or mixed.
Preferred polyarylene ether sulfones in one embodiment include carboxyl-containing polyarylene ether sulfones with recurring structural elements of the formulae I and II
where the variables are as defined above and R
1
is H, C
1
-C
6
-alkyl or —(CH
2
)
n
—COOH, in particular mixed with polyarylene ether sulfones which contain inert groups and where
x is 0.5

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