Multilayer composite comprising layers of partly aromatic polyamides

Patent metadata

Field	Value
Publication number	US-10464296-B2
Application number	US-201615072891-A
Country	US
Kind code	B2
Filing date	Mar 17, 2016
Priority date	Mar 17, 2015
Publication date	Nov 5, 2019
Grant date	Nov 5, 2019

Abstract

A multilayer composite containing the following layers: 1. a first layer (layer I) of a moulding compound containing at least 40 wt. % of the following components: 1) 60 to 99 parts by wt. of a copolyamide based on hexamethylenediamine, terephthalic acid and an aliphatic dicarboxylic acid having 8 to 19 carbon atoms and 2) 40 to 1 parts by wt. of an olefinic copolymer as impact modifier, wherein the parts by wt. of 1) and 2) sum to 100; and II. a second layer (layer II) of a moulding compound containing at least 60 wt. % of a mixture of the following components: 1) 75 to 100 parts by wt. of a partly aromatic copolyamide and 2) 25 to 0 parts by wt. of an olefinic copolymer as impact modifier with the proviso that in the moulding compound of layer II the mixture of components 1) and 2) comprises at least 5 fewer parts by wt, of olefinic copolymer than in the moulding compound of layer I, has a high heat distortion temperature, a very good impact resistance, a high elongation at break and good layer adhesion.

First claim

The invention claimed is:

1. A multilayer composite, comprising the following layers:
I. a first layer (layer I) of a moulding compound comprising at least 40 wt. % of the following components:
1) 60 to 95 parts by wt. of a copolyamide comprising as copolymerized monomer units:
α) 45 to 90 mol % of a combination of hexamethylenediamine and terephthalic acid, and
β) 55 to 10 mol % of a combination of hexamethylenediamine and a linear aliphatic dicarboxylic acid having 8 to 19 carbon atoms;
wherein the mol % values relate to the sum of α) and β), and
Wherein not more than 20% of the hexamethylenediamine is optionally replaced by the equivalent amount of another diamine, and/or
wherein not more than 20% of the terephthalic acid is optionally replaced by the equivalent amount of another aromatic dicarboxylic acid and/or 1,4-cyclohexanedicarboxylic acid, and/or
wherein not more than 20% of the repeating units containing hexamethylenediamine and linear aliphatic dicarboxylic acid is optionally replaced by the equivalent quantity of units obtained from a lactam/an ω-aminocarboxylic acid having 6 to 12 carbon atoms,
2) 40 to 5 parts by wt. of an olefinic copolymer as impact modifier, the olefinic copolymer comprising:
35 to 94.9 wt % ethene,
5 to 64.9 wt % of a 1-alkene having 4 to 8 carbon atoms,
0 to 10 wt % of monomer units of an olefin different from ethene and the 1-alkene having 4 to 8 carbon atoms, and
0.1 to 2.5 wt % of monomer units based on an aliphatically unsaturated dicarboxylic anhydride,
Wherein the individual wt % values of the olefinic copolymer sum to 100;
wherein the parts by wt. of 1) and 2) sum to 100; and
II. a second layer (layer II) comprising at least 60 wt. % of a mixture of the following components:
1) 75 to 100 parts by wt. of a partly aromatic copolyamide, and
2) 25 to 0parts by wt. of an olefinic copolymer as impact modifier;
wherein layer I is in direct contact with layer II, and
with the proviso that in the moulding compound of layer II the mixture of components 1) and 2) comprises at least 5 fewer parts by wt. of olefinic copolymer than in layer I; and
wherein the partly aromatic copolvamide of layer II is the same as the copolyamide of layer I.

2. The multilayer composite according to claim 1 , wherein the moulding compound of layer I further comprises 0.01 to 60 wt. % of an additive.

3. The multilayer composite according to claim 2 , wherein the additive is a copper-containing stabilizer.

4. The multilayer composite according to claim 2 , wherein the additive is an oxidation stabilizer.

5. The multilayer composite according to claim 1 , wherein a crystallite melting point T m of the copolyamide of layer I is from 220° C. to 300° C. when measured as per ISO 11357 at 2nd heating.

6. The multilayer composite according to claim 1 , which further comprises at least one more layer.

7. The multilayer composite according to claim 6 , wherein the at least one more layer is selected from the group consisting of
a further layer I,
a further layer II,
a layer of a moulding compound based on an aliphatic polyamide,
a layer of a moulding compound based on a fluoropolymer,
a layer of an EVOH moulding compound, and combinations thereof.

8. The multilayer composite according to claim 6 , wherein the at least one more layer is the same as the first layer (I).

9. The multilayer composite according to claim 1 , which is a film, a sheet or a hollow article.

10. The multilayer composite according to claim 9 , which is a hollow article and wherein the hollow article is a hollow profile.

11. The multilayer composite according to claim 10 , which further comprises a layer selected from the group consisting of an electrically conductive layer, an elastomer sheathing and combinations thereof.

12. The multilayer composite according to claim 10 , wherein the hollow profile is selected from the group consisting of a fuel line, a hydraulic line, a brake line, a clutch line, a coolant line, a liner for rigid or flexible pipes in the oil or gas extraction industry and a line for an umbilical.

13. The multilayer composite according to claim 10 , wherein the hollow profile is a brake fluid container or a fuel container.

14. The multilayer composite according to claim 10 , wherein the hollow profile is a pipe, or a container.

15. The multilayer composite according to claim 1 , wherein the second layer (layer II) does not comprise an olefinic copolymer.

16. The multilayer composite according to claim 1 , wherein the 1-alkene is selected from the group consisting of 1-butene, 1-pentene, 4-methylpent-1-ene and 1-hexene.

17. A multilayer composite, comprising the following layers:
I. a first layer (layer I) of a moulding compound comprising at least 40 wt. % of the following components:
1) 60 to 95 parts by wt. of a copolyamide comprising as copolymerized monomer units:
α) 45 to 90 mol % of a combination of hexamethylenediamine and terephthalic acid, and
β) 55 to 10 mol % of a combination of hexamethylenediamine and a linear aliphatic dicarboxylic acid having 8 to 19 carbon atoms;
wherein the mol % values relate to the sum of α) and β), and
wherein not more than 20% of the hexamethylenediamine is optionally replaced by the equivalent amount of another diamine, and/or
wherein not more than 20% of the terephthalic acid is optionally replaced by the equivalent amount of another aromatic dicarboxylic acid and/or 1,4-cyclohexanedicarboxylic acid, and/or
wherein not more than 20% of the repeating units containing hexamethylenediamine and linear aliphatic dicarboxylic acid is optionally replaced by the equivalent quantity of units obtained from a lactam/an ω-aminocarboxylic acid having 6 to 12 carbon atoms,
2) 40 to 5 parts by wt. of an olefinic copolymer as impact modifier, the olefinic copolymer comprising:
35 to 94.9 wt % ethene,
5 to 64.9 wt % of a 1-alkene having 4 to 8 carbon atoms,
0 to 10 wt % of monomer units of an olefin different from ethene and the 1-alkene having 4 to 8 carbon atoms, and
0.1 to 2.5 wt % of monomer units based on an aliphatically unsaturated dicarboxylic anhydride,
wherein the individual wt % values of the olefinic copolymer sum to 100;
wherein the parts by wt. of 1) and 2) sum to 100; and
II. a second layer (layer II) consisting of a partly aromatic copolyamide;
wherein layer I is in direct contact with layer II and wherein the partly aromatic copolyamide of layer II is the same as the copolyamide of claim I.

18. The multilayer composite according to claim 17 , wherein the moulding compound of layer I further comprises 0.01 to 60 wt. % of an additive.

19. The multilayer composite according to claim 18 , wherein the additive is a copper-containing stabilizer.

20. The multilayer composite according to claim 18 , wherein the additive is an oxidation stabilizer.

21. The multilayer composite according to claim 17 , wherein a crystallite melting point T m , of the copolyamide of layer I is from 220° C. to 300° C. when measured as per ISO 11357 at 2nd heating.

22. The multilayer composite according to claim 17 , which further comprises at least one more layer.

23. The multilayer composite according to claim 22 , wherein the at least one more layer is selected from the group consisting of
a further layer I,
a further layer II,
a layer of a moulding compound based on an aliphatic polyamide,
a layer of a moulding compound based on a fluoropolymer,
a layer of an EVOH moulding compound,

Assignees

• Berger Jasmin
• Goering Rainer
• Kuhmann Karl
• Evonik Degussa Gmbh

Inventors

• Berger Jasmin
• Goering Rainer
• Kuhmann Karl

Classifications

• C08G69/265

  from at least two different diamines or at least two different dicarboxylic acids · CPC title

• C08L77/06

  Polyamides derived from polyamines and polycarboxylic acids (C08L77/10 takes precedence) · CPC title

• C08L77/02

  Polyamides derived from omega-amino carboxylic acids or from lactams thereof (C08L77/10 takes precedence) · CPC title

• C08L51/04

  grafted on to rubbers · CPC title

• C08K5/098

  Metal salts of carboxylic acids · CPC title