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Patent 1270979 Summary

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(12) Patent: (11) CA 1270979
(21) Application Number: 426555
(54) English Title: POLYETHERIMIDE-POLYAMIDE BLENDS
(54) French Title: MELANGES DE POLYETHERIMIDE-POLYAMIDE
Status: Deemed expired
Bibliographic Data
(52) Canadian Patent Classification (CPC):
  • 400/5804
  • 400/7830
(51) International Patent Classification (IPC):
  • C08L 79/08 (2006.01)
  • C08L 77/02 (2006.01)
  • C08L 77/06 (2006.01)
(72) Inventors :
  • GILES, HAROLD F., JR. (United States of America)
  • WHITE, DWAIN M. (United States of America)
(73) Owners :
  • GILES, HAROLD F., JR. (Not Available)
  • WHITE, DWAIN M. (Not Available)
  • GENERAL ELECTRIC COMPANY (United States of America)
(71) Applicants :
(74) Agent: OLDHAM AND WILSON
(74) Associate agent:
(45) Issued: 1990-06-26
(22) Filed Date: 1983-04-22
Availability of licence: N/A
(25) Language of filing: English

Patent Cooperation Treaty (PCT): No

(30) Application Priority Data: None

Abstracts

English Abstract






POLYETHERIMIDE-POLYAMIDE BLENDS
ABSTRACT OF THE DISCLOSURE
Disclosed are blends comprising from about
40 to 80 wt. % of a polyetherimide and the remainder one
or more polyamides. The blends generally have a tensile
strength which is greater than the tensile strength of
polyetherimide-polyamide blends which do not contain from
about 40 to 80% polyetherimide, while still retaining a
good combination of other physical properties such as
heat distortion characteristics and impact strength. In
addition, the blends of the invention may have a flexural
strength which is greater than that of other polyether-
imidepolyamide blends which do not contain from about
40 to 80% polyetherimide. The blends of the present
invention find use in automobile and aviation
applications for decorative and protective purposes and
in high temperature electrical insulation applications.


Claims

Note: Claims are shown in the official language in which they were submitted.



- 22 - 8CU 3456
The embodiments of the invention in which an
exclusive property or privilege is claimed are defined
as follows:
1. A composition comprising a blend of
(a) a polyetherimide and (b) a polyamide wherein the
polyetherimide comprises about 40% to about 70%
of the blend by weight wherein the polyetherimide has
the formula
Image
where a represents a whole number in excess of 1, the
group Image selected from:
Image
R1 being hydrogen, lower alkyl or lower alkoxy, Z is a
member of the class consisting of (1)
Image


- 23 - 8CU 3456
Claim 1 continued:
Image
and (2) divalent organic radicals of the general formula:
Image
where X is a member selected from the class consisting
of divalent radicals of the formulas,
-CyH2y-, ?, Image, -O- and -S-
where q is 0 or 1, y is a whole number from 1 to 5,
and R is a divalent organic radical selected from the
class consisting of (1) aromatic hydrocarbon radicals
having from 6-20 carbon atoms and halogenated derivaties
thereof, (2) alkylene radicals and cycloalkylene radicals
having from 2-20 carbon atoms, and C(2-8) alkylene
terminated polydiorganosiloxane, and (3) divalent radicals
included by the formula
Image
where Q is a member selected from the class consisting of
- O- , ? , Image , -S- and -CxH2x
where x is a whole number from 1 to 5 inclusive.


- 24 - 8CU 3456

2. A composition in accordance with claim 1
wherein the polyetherimide comprises from about 40% to
about 60% of the blend by weight.
3. A composition in accordance with claim 2
wherein the polyetherimide is of the formula:
Image
and the divalent bonds of the -O-Z-O- radical being in
the 3,3'; 3,4'; 4,3' or the 4,4' position.
4. A composition in accordance with claim 1
wherein the polyetherimide is of the formula:
Image
and the divalent bonds of the -O-Z-O- radical being in
the 3,3'; 3,4'; 4,3' or the 4,4' position.
5. A composition in accordance with claim 3
wherein Z is:
Image


- 25 - 8CU 3456
and R is selected from:
Image .
6. A composition in accordance with claim 4
wherein Z is:
Image
and R is selected from:
Image .
7. A composition in accordance with claim 5
wherein the polyetherimide is of the formula:
Image .
8. A composition in accordance with claim 6
wherein the polyetherimide is of the formula:


- 26 - 8CU 3456
Image .
9. A composition in accordance with claim 1
wherein the polyamide has repeating structural units of
the formula:
Image
wherein R2, R3 and R4, which may be the same or
different, each represents an alkylene group having from
4 to 11 carbon atoms, and n is an integer of 30 to 500 or
more.
10. A composition in accordance with claim 2
wherein the polyamide has repeating structural units of
the formula:
Image
wherein R2, R3 and R4, which may be the same or
different, each represents an alkylene group having from
4 to 11 carbon atoms, and n is an integer of 30 to 500 or
more.
11. A composition in accordance with claim 3
wherein the polyamide has repeating structural units of
the formula:


- 27 - 8CU 3456
Image
wherein R2, R3 and R4, which may be the same or different,
each represents an alkylene group having from 4 to 11
carbon atoms, and n is an integer of 30 to 500 or more.
12. A composition in accordance with claim 4
wherein the polyamide has repeating structural units of the
formula:
Image
wherein R2, R3 and R4, which may be the same or different,
each represents an alkylene group having from 4 to 11
carbon atoms, and n is an integer of 30 to 500 or more.
13. A composition in accordance with claim 5
wherein the polyamide has repeating structural units of the
formula:
Image
wherein R2, R3 and R4, which may be the same or different,
each represents an alkylene group having from 4 to 11
carbon atoms, and n is an integer of 30 to 500 or more.
14. A composition in accordance with claim 6
wherein the polyamide has repeating structural units of the
formula:
Image


- 28 - 8CU 3456
wherein R2, R3 and R4, which may be the same or different,
each represents an alkylene group having from 4 to 11
carbon atoms, and n is an integer of 30 to 500 or more.
15. A composition in accordance with claim 7
wherein the polyamide has repeating structural units of the
formula:
Image
wherein R2, R3 and R4, which may be the same or different,
each represents an alkylene group having from 4 to 11
carbon atoms, and n is an integer of 30 to 500 or more.
16. A composition in accordance with claim 8
wherein the polyamide has repeating structural units of the
formula:
Image
wherein R2, R3 and R4, which may be the same or different,
each represents an alkylene group having from 4 to 11
carbon atoms, and n is an integer of 30 to 500 or more.
17. A composition in accordance with claim 9, 10
or 11 wherein the polyamide is nylon 66.
18. A composition in accordance with claim 12,13
or 14 wherein the polyamide is nylon 66.
19. A composition in accordance with claim 15 or
16 wherein the polyamide is nylon 66.
20. A composition in accordance with claim 1
wherein the polyamide is nylon 66.
21. A composition in accordance with claim 9, 10
or 11 wherein the polyamide is nylon 12.
22. A composition in accordance with claim 12,
13 or 14 wherein the polyamide is nylon 12.


- 29 - 8CU 3456

23. A composition in accordance with claim 15
or 16 wherein the polyamide is nylon 12.

Description

Note: Descriptions are shown in the official language in which they were submitted.


~2~7~




- 1 - 8CU-3456

POLYETHERI~IDE-POLYAMIDE BLENDS
-
The invention relates to a particular class of
polyetherimide-polyamide blends where the blend contains
from 40 to 80 wt. % polytheri~ide~;~- .Among other things,
such blends have a hi~her tensile strength than those
associated wit~ polyetherimide-polyamides blends contain-
ing less t~an ~0% polyetherimide and some.blends containing
more than 80% polyethermide.
The blends o~ the invention include a polyetherimide
o~ the formula:

o_z_O~


O o


whexe a represents a whole number in excess af 1~ e.g.,
10 to 10,000 or more, the group.-O-A = is selected from:




' ~ ~

.,. ~.


:~ .; . .: , , :. : .. , '';,, ','. ;

~L2~37~
` 8CU-3456




S _~ ~

" _ I

R' being hydrogen, lower alkyl or lower alXoxy, prefer~bly
the polyetherimide includes the latter -O-A group
1~ where R' is hydrogen such that the polyether~mide lS
of the formula: .


O. -
~o - o ..
n

t f \ -- -- O ~ / N R t

~5 " a
O O



and the divalent bonds of tbe -O-Z-O-radical are in
the 3,3';3,4';4,3' or the 4,4' position;
and Z is a member of the class consisting of (11
~ .

.

. .: . , ::
~ ,, . ,. ~ ,. ~ , . -
,- : . .. , -. ~: .. ..

' '` ''~ . ' '. ' "" ' ' ,. ' '; . ' ` ' ' ' " " ' '' '
'~' ~.'. ''.' .1 ,. ' , , `.

~7~?~7~

8CU-3456
-- 3 --
.

- ~/3 ~`
~If~ ~



l~ ~ ~ C(C~3)~


and (2~ divalent organic radicals of -the general formula:


` {O} tX) ~0}

.
where X is a member selected from the class consisting
o~ divalent radicals of the formulas,
O O
CyH2y C - , S - - O - and - S -
o




where q is O or 1, y is a whole number from 1 to 5, and

R is a divalent organic radical selected from the class

consisting of (11 aromatic hydrocarbon radicals having

from 6-20 carbon atoms and halogenated derivatives

thereof, (2~ alkylene ra~icals and cycloalkylene radicals

having from 2-20 carbon atoms, C(2 8~ alkylene terminated

polydiorganosiloxane, and (31 divalent radicals included




,. ~

-. -:



.~ . . . .



, . . .



.. . .



.:.. ,, .,.:.. . ~: ., .


'' ' :: ,

~7~
8CU-3456
~ 4
by the formula


~ ~ Q - ~ .

where Q is a member selected from the class conslsting of
O O

- O - - C ~ - S ~ - S - and - C~H2


where X is a whole number from 1 to 5 inclusive. Par-
ticularly preferred polyetherimides for the purposes of
the present invention include those where - O - A- and
15 ~ r~Spectively are: CH3

- O ~ and CO } ~ -

7~)

and R is selected from:



--~'CH2 ~ (~ (~



The polyetherimides where R is metaphenylene are most



. . . . . ................ ~ ... ~ .


: . ; .:., .

~Z7~

8CU-3456
-- 5 --

preferred.
As mentioned previously, the hlends of the invention
also include a polyamide. Polyamides are well known in
the art and the term embraces those semi-crystalline and
amorphous resins having a molecular weight of at least
5000 commonly referred to as nylons. Polyamides generally
have a repeating structual units represented by the
general formula;

1~ ~ O H

t N ~ or t C - R3~ C - N - R - N

1~
where R2, R3r and R4, which may be the same or different,
each represents an alkylene group having from 4 to 11
carbon atoms, and n is an integer of 30 to 500 or more.
Suitable examples of alkylene groups containing 4 to 11
~o carbon atoms for R2, R3, and R4 include a
tetramethylene group, a pentamethylene group, a
hexamethylene group, a heptamethylene group, an
octamethylene group, a nonamethylene group, decamethylene
group, an undecamethylene group, and the like.
~5 Specif~cally, the following polyamides may be
incorporated in the blends of the invention:
polyhexamethylene adipamide (nylon 6;6)
polypyrrolidone (nylon 4)
polycaprolactam (nylon 6)
polyheptolactam (nylon 7)
polycapryllactam (nylon 81
polynonanolactam ~nylon 9
polyundecanolactam (nylon 11
polydodecanolactam (nylon 12
polyhexamethylene azelaiamide (nylon 6:9~
polyhexamethylene sebacamide (nylon 6010)




:: ~ - , ; : :, : :- :, - , ::: .

~n~7~
8CU-3~56
-- 6

polyhexamethylene isophthalamide (nylon 6:ip)
polymetaxylylene adipamide (nylon MXD:6)
polyamide ~ hexamethylenedediamine and n-dodecanedioic
acid (nylon 6:12~
polyamide of dodecamethylenediamine and
n-dodecanedioic acid (nylon 12:12)
Nylon copolymers may also be used as the polyamide
component of the blends of this invention. For example,
suitable copolymers include the following:
hexamethylene adipamide/caprolactam (nylon 6:6/6)
hexamethylene adipamide/hexamethylene-isophthalamide
~nylon 6:6~6ip~
hexamethylene adipamide/hexamethylene-terephthalamide
(nylon 6:6/6T~
trimethylhexamethylene oxamide/hexamethylene oxamide
(nylon trimethyl-6:2/6:2~
hexamethylene adipamide/hexamethylene-azelaiamide
~nylon 6:6/6:9)
hexamethylene adipamide/hexamethylene-azelaiamide/
caprolactam (nylon 6:6/6:9/6)
Also useful is nylon 6:3 produced by Dynamit Nobel.
This polyamide is the product of the dimethyl ester of
terephthalic acid and a mixture of isomeric trimethyl
hexamethylenediamine. Preferred nylons for the blends
of the invention include 6,6/6; 11,/6/3 and 6/12.
In addition, specific polyamides are described
in U.S. Patent Nos~2,071,.250; 2,071,251; 2,130,523;
,130,948; 2,241,322; 2,312,966; 2,512,606 to Bolton
dated June 27, 19.50 and 3,393,210 to Speck dated
July 16, 1968.
The polyetherimides can be obtained by any of the
methods well known to those skilled in the art including
the reaction of ~ny ar~matic bis (ether anhydrides) of
the formula


: ~`


. .. ,: ...................... .

D7~
8CU-3456
- 7 -

. O
/C\[~ - Z


where 2 is as defined hereinbefore with an organic diamine
of the formula
H2N-R-NH2

where R is as defined hereinbefore.
Aromatic bis(ether anhydride)s of the above formula
include, for example, 2,2-bisl4-(2,3-
dicarboxyphenoxy~phenyl]-propane dianhydride; 4,4'-bis(2,
3-dicarboxyphenoxy~diphenyl ether dianhydride; 1,3-bis(2,
dicarboxyphenoxy~diphenyl sulfide dianhydride; 1,4-bi 5( 2,
3-dicarboxyphenoxy~benzene dianhydride; 4,4'-bis(2,3-
dicarboxyphenoxy~benzophenone dianhydride; 4,4'-bis
(~,3-dicarboxyphenoxyldiphenyl sulfone dianhydride;
2-bis[4-(3,4-dicarboxyphenoxy)phenyl]propane dianhydride;
4,4'-bis(3,4-dicarboxyphenoxy~diphenyl ether dianhydride;
~,4'-bis(3,4-dicarboxyphenoxy)diphenyl sulfide dianhydride;
1,3-bis(3,4-dicarboxyphenoxy)benzene-dianhydrlde;
1,4-bis(3,4-~iaarboxyphenoxy)benzene~dianhydride;~
~5 ~,4`-bis(3,4-dicarboxypheno-xy)benzophenone dianhydride;
4-(2,3-dicarboxyphenoxy~-4'(3,4-dicarboxyphenoxy)diphenyl
2,2-propane dianhydride; etc., and mixtures of such
dianhydrides.
In addition, aromatic bis(ether anhydride)s also
included by the above formula are shown by Koton, M~M.;
Florinski, F.S.; Bessonov, M.I.; Rudakov, A.P. (Institue
of Heteroorganic compounds, Academy of Sciences, U.S.S.R.),
U.S.S.R. 257,010, Nov. 11, 1969, Appl. May 3, 1967. In
~ddition, dianhydride~ are shown by M.M. Koton, F.S.
35 Florinski, Zh Org. Khin, 4(5~, 774 (1968).

.

~;~7~7~
8CU-3456
-- 8

Organic diamines of the above formula include, for
example, m-phenylenediamine, p-phenylenediamine, 4,4'-
diaminodiphenylpropane, 4,4'-diaminodiphenylmethane,
benzidine, 4,4'-diaminodiphenyl sulfide,
5 4,4'-diaminodiphenyl sulfone, 4,4'-diaminodiphenyl ether,
1,5-diaminonaphthalene, 3,3'-diaminodiphenyl ether,
1,5-diaminonaphthalene, 3,3'-dirnenthylbenzidine !
3,3'-dimethoxybenzidine, 2,4-bis,P -amino-t-butyl)toluene,
bis~p- ~ -amino-t-butylphenyl) ether, bis (p-7~- methyl-o-
aminopentyl)benzene, 1,3-diamino-4-isopropylbenzene,
1,2-bis~3-aminopropoxy~ethane, m-xylylenediamine,
p-xylylened~amine, 2,4-diaminotoluene, 2,6-diaminotoluene,
bis(4-aminocyclohexyl)methane, 3-methylheptamethylene-
diamine, 4,4-dimethylheptamethylenediamine,
15 2,11-dodecanediamine, 2,2-dimethylopropylenediamine,
octamethylenediaminer 3-methoxyhexamethylenediamine,
2,5-dimethylhexamethylenediamine,
~,5-dimethylheptamethylenediamine,
3-methylheptamethylenediamine,
20 5-methylnonamethylenedediamine, 1,4-cyclohexanediamine,
1,12-octadecanediamine, bis(3-aminopropyl~sulfide,
N-methyl-bis~3-aminopropyl)amine, hexamethylenediame,
lleptamethylenediamine, nonamethylenediamine,
decamethylenediamine, bis(3-aminopropyl)
tetramethyldisiloxane, bis (4-aminobutyl~
tetramethyldisiloxane, and the like.
In general, the reactions can be advantageoulsy
carried out employing well-known solvents, e.g.,
o~dichlorobenzene, m-cresol/dianhydrides and the diamines,
30 at temperatures of from about 100 to about 250C. Altern-
atively, the polyetherimides can be prepared by melt poly-
merization of any of the above dianhydrides with any of
the above diamine compounds while heating the mixture
of the ingredients at elevated temperatures with
35 cc~ncurrent intermixing. Generally, melt polymerization
temperatures between about 200 to 400C. and preferably



., : , . ~ : , . . . ;
. . " :. ,

- : . :, ~ .- . :. : :
~"~

~7q:~7~3

8CU-3456
g

230 to 300C. can be employed. The conditions of the
reaction and the properties of ingredients can be varied
widely depending on the desired molecular weight, intrinsic
viscosity, and solvent resistance. In general, equimolar
amounts of diamine and dianhydride are employed for high
molecular weight polyetherimides, however, in certain in-
~tances, a slight molar excess (about 1 to 5 mol percent)
of diamine can be employed resulting in the production of
polyetherimides having terminal amine groups. Generally,
useful polyetherimides ha~e an intrinsic viscosity greater
than 0.2 deciliters per gram, preferably 0.35 to 0.60, or
0.7 deciliters per gram or even higher when measured in
m-cresol at 25C.
Included among the many methods of making the poly-

etherimides are those disclosed in U.S. Patent Nos.Heath et al, 3,847,867 dated November 12,1974, Williams
3,8~7,869 dated November 12, 1974, Takehoshi et al,
3,850,885 dated Noyember 26, 1974, White 3,852,242 dated
December 3, 1974 and 3,855,178 dated December 17, 1974.
These disclosures teach general and specific methods
for preparin~ polye`therimides suitable for the blends of
this invention.
Polyamides may be obtained by polymerizing a
monoaminomonocarboxylic acid or an internal lactam thereof
~avin~ at least t~o carbon atoms between the amino and
carboxylic acid groups; or by polymerizing substantially
equimolar proportions of a diamine which contains at least
t~o carbon atoms between the amino groups and a dicar-
boxylic acid; or by polymerizing a monoaminocarboxylic
acid or an internal lactam thereof as defined above
together with substantially equimolecular proportions of
a diamine and a dicarboxylic acid. The dicarboxylic acid
may be used in the from of a functional derivative thereof,
for example, an ester.
The term "substantially equimolecular proportions"
(o~ the diamine and of the dicarboxylic acid) is used to



. .

7 ~ ~ 7 ~
8CU-3456
-- 10 --

comprehend both strict equimolecular proportions and the
slight departures therefrom which are in~olved in
conventional techniques for stabilizing the ~iscosity of
the resultant polyamides.
As examples of the monoaminomonocarboxylic acids or
lactams thereof, there may be mentioned those compounds
containing from 2 to 16 carbon atoms between the amino
an~ carboxylic acid groups, the carbon atoms forming a
rill~ with the -CO-NH- group in the case of a lactam. As
particular examples of aminocarboxylic acids and lactams
there may be mentioned ~ -aminocaproic acid, butyrolactam,
pivalolactam, caprolactam, capryl-lactam, enantholactam,
undecanolactam, dodecanolactam and 3- and 4-amino benzoic
acids.
Examples of suitable diamines are diamines of the
~ene~al formula H2N(CH2~nNH2 wherein n is an integer of
from ~ to 16, such as trimethylenediamine, tetramethyl-
enediamine, pentamethylenediamine, octamethylenediamine,
decamethylenediamine, dodecamethylenediamine, hexade-
camethylenediamine, and especially hexamethylenediamine.
C-alkylated diamines, e.g., 2,2-dimethylpentamethylene-
diamine and 2,2,4-and~2,4,4-trimethylhexamethylenediamine
~re further examples. Other diamines which may be mentioned
~s examples are aromatic diamines, e.g., p-phenylenediamine,
~,4'-diaminodiphenyl sulfone, 4,4'-diaminodiphenyl ether
and 4,4'-diaminodiphenyl sulfone, 4,4'-diaminodiphenyl
ether and 4,4'-diaminodiphenylmethane; and cycloaliphatic
diamines, for example, diaminodicyclohexylmethane.
The dicarboxylic acids may be aromatic, for example,
3~ isophthalic and terephthalic acids. Preferred dicar-
boxylic acids are of the formula HOOC-Y-COOH wherein Y
presents a divalent aliphatic radical containing at least
two carbon atoms, and examples of such acids are sebacic
acid, octadecanedioic acid, suberic acid, azelaic acid,
undecanedioic acid, glutaric acid, pimelic acid, and
especially adipic acid. Oxalic acid is also a preferred

8CU-3~56
-- 11 --
acid.
As was mentioned previously, the blends of the present
invention comprise from about 40 to 80 wt. % preferably
from 40 to 60 wt. % of a polyetherimide and the remainder
one or more polyamides. Such blends generally have a
tensile strength which is greater than the tensile strength
of polyetherimide-polyamide blends which do not contain
from 40 to 8Q% polyetherimide, while still retaining a
good combination of other physical properties such as
heat distortion characteristics and impact strength. In
addition, the blends of the invention may have a flexural
strength which is greater than that of polyetherimide-
polyamide blends outside the scope of the invention.
Consequently, by controlling the proportions of the poly-
etherimide and po-lycarbonate relative to each other within
the above range, it was surprisingly found that blends
having properties which are improved over those of blends
outside the range as well as over the polyetherimide or
polyamide components alone can be achieved. Thus, the
i~o blends of the invention provide materials which have certain
properties approaching those of the polyetherimide component
~l~ne while contalning a significant proportion of the
generally presently less expensive polyamide relative to
the polyetherimide. Furthermore, blends within the
composition range of the present invention have an appearance
which suggests that the blends are of one phase and there
fore compatible.
The unlque characteristics of the blends of the pre-
sent invention are illustrated ln the drawings in which;
Figure 1 is a plot of unnotched impact strength versus
polyetherimide content for blends of a polyetherimide and
a polyamide,
Figure 2 is a plot of heat distortion temperature
versus polyetherimide content for blends of a polyetherimide
and a polyamide,
Figure 3 is a plot of ultimate flexural strength versus

~ ,~




,, ",, ' ' ,. :,, , ! ~ `
': ,

7~97~
8CU-3456
- 12 -

polyetherimide content for blends of a polyetherlmide
and a polyamide,
Figure 4 is a plot of flexural modulus versus poly-
etherimide concentration for blends of a polyetherimide
and a polyamide, and
Figure 5 is a plot of tensile strength versus poly-
etherimide concentration for blends of a polyetherimide
~nd a polyamide.
It is contemplated that the polyetherimide-polyamide
blends of the present invention may also include other
additives materials such as fillers, stabilizers, plastici-
zers, fle~ibilizers, surfactant agents, pigments, dyes,
reinforcements, flame retardants and diluents in conven-
tional amounts. It is also contemplatea that the blends
of the in~ention may include two or more polyetherimides
with one or more polyamides or two or more polyamides in
combination w~th one or more polyetherimides.
Methods for forming polyetherimide-polyamide blends
may vary considerably. Prior art blending techniques
~o are generally satisfactory. A preferred method comprises
blending the polymers and additives such as reinforcements
in power, granular or ~ilamentous form, extruding the
blend/ and chopping the extrudate into pellets suitable for
moldin~ by means con~entionally used to mold normally solid
thermoplastic compositions.
The particular polyetherimide-polyamide blends of the
present invention have application in a wide variety of
physical shapes and forms, including the use as films,
molding compounds, coatings, etc. When used as films or
when made into molded products, these blends, including
laminated products prepared therefrom, not only possess
good physical properties at room temperature but they
train their strength and excellent response to workloading
at elevated tempexatures for long periods of time. Films
~ormed from the blends of this invention may be used in
application where films have been used previously. ThUs~the



,. , ..


- , ., .. , . : :. :

8CU-3456
- 13 -
blends of the present invention can be used in automobile
and aviation applications for decorative and protective
purposes, and as high temperature electrical insulation
for motor slot liners/ transformers, dielectric capacitors,
cable and coil wrappings (form wound coil insulation for
motors~, and for containers and container linings. ~he
blends can also be used in laminated structures where
films or solutions of the blend are applied to ~arious
heat-resistant or other type of materials such as asbestos,
mica, ~lass fiber and the like, the sheets super-imposed
one upon the other, and thereafter subjecting the
sheets to elevated temperatures and pressures to effect
flow and cure of the resinous binder to yield cohesive
laminated strcutures. Films made from the subject poly-
l~ etherimide-polyamide blends can also serve in printed
circuit applications.
Alternatively, solutions of the blends herein des-
cribed can be coated on electrical conductors such as
copper, aluminum, and the like and thereafter the coated
conductor can be heated at elevated temperatures to remove
the solvent and to form a continuous coating of the re-
sinous composition thereof. If desired, an additional
overcoat may be applied to such insulated conductors
includin~ the use of polymeric coatings, such as poly-
amides, polyesters, silicones, polyvinylformal resins,
epo~y resins, polyimides, polytetrafluorethylene, etc.
The use of the blends of the present invention as overcoats
on other types of insulation is not precluded.
Other applications which are contemplated for these
blends include their use as binders for asbestos fibers,
carbon iberst and other fibrous materials in making brake
linings. In addition, molding compositions and molded
articles may be formed from the polymeric blends of the
in~ention such as by incorporating such fillers as asbestos,
glass fibers, tàlc, ~uartz, powder, finely divided carbon,
silica, and the like into the blends prior to molding.




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8CU-3456
- 14 ~

~naped articles may be formed under heat, or under heat
and pressure, in accordance with practices well-known in
the art.
The following examples illustrate specific poly-
etherimide-polyamide blends in accordance with the pre-
sent invention. It should be understood that the
examples are given for the purpose of illustration and
do not limit the invention. In the examples, all parts
alld percentages are by weight unless otherwise specified.
1~
Example I
A series of polyetherimide-nylon 6:6 blends, some
according to the inYention and some outside the invention,
were prepared, the hlends molded into test specimens and
the specimens tested for various physical properties.
1~ The polyetherimide of the blends was prepared from
the reaction product of essentially equimolar amounts of
2,2-bis~4-(3,~-dicarboxy phenoxy~phenyl] propane dianhy-
dride and m-phenylene diamine produced at elevated
temperature of about 250 to about 300C. and under a
nitrogen atmosphere. The polymer was extruded at about
300C. to form a strand and mechanically chopped into
pellets. A test specimen of the polyetherimide was
injection molded from the pellets at a temperature of
about 685-700F. The physical properties of the poly-
etherimide are set forth in the first line of the following
Table I.
The polyamide used in preparing the blends was a
general purpose nylon 6:6 sold under the tradename
Vydyne 21X by Monsanto Chemical Co. This polyamide alone
has the properties set forth at the bottom of Table I.
About ~0 parts of the above polyetherimide were mixed with
about lQ parts of the polyamide. The mixture of the7rt~wo
; polymers was then extruded in a Werner & Pfleiderer extruder
havin~ a temperature profile varying from about 226 to




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8CU-3456
- 15 -

326C and a die temperature of about 316C. The resulting
extrudate was comminuted into pellets and the pellets
- injection molded into test specimens in a sattenfield ~
molding machine at a temperature of about 265C to 321C.
The impact strength of these specimens were measured
according to the unnotched and notched Izod impact test
and the results are set forth in the following Table I.
The heat distoration temperature, flexural properties,
tensile properties and appearance of the blend were
also determined and are given in Table I.
The above procedure for preparing the blend was then
repeated to produce test specimens of three additional
blends having varying amounts of polyetherimide relative
to the polyamide. The results of the unnotched and
notched Izod impact test, as well as the heat distortion
temperature, flexural properties, tensile properties and
~ppearance for thes lends are also detailed in Table I.




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8CU-3456
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In Figures 1-5, some of the data from Table I is
plotted versus relative concentration of the components
of the blends in solid lines. From Figure 1, a plot of
the unnotched Izod impact strength versus polyetherimide
concentration, it can be observed that small amounts of
nylon result in significantly lower unnotched impact
strength values. However, af~er this initial drop, the
impact values remain relatively constant to the 50:50
~lend level before another small decrease is observed.
The notched Izod impact strength values are somewhat
similar to the unnotched values. The notched impact
strength of the blends decreased from pure polyetherimide
to the 70% polyetherimide blend level and then remains
~airly constant regardless of the blend ratio. From
Figure 2, it is apparent that the heat distortion tem-
perature values decrease only slightly from 100% poly-
etherimide to 70% concentrations of polyetherimide, but
beyond this point the heat distortion temperature drops
a~out 30C. to 140C. where it remains generally constant
oyer the rema~nder of the blend compositions tested.
The flexural properties are plotted in Figures 3 an
~. The flexural strength decreases very rapidly from the
100~ polyetherimide to 90% blend level and then increases
slightly to a maximum occurring at about a 50:50 blend
ratio as is shown in Figure 3. In Figure ~, the flexural
modulus can be seen to decrease as nylon is initially
added, then level out, and decrease again as the ccncen-
tration of polyetherimide in the blends if reduced below
about 50%.
From Figure 5, the plot shows that the tensile failure
strength decreases substantially at the 10% nylon blend
level from the pure polyetherimide level but then the
strength`increases to a maximum at about the 50:50 blend
level`where it is only about 6% lower than the tensile
failure strength of the polyetherimide. The substantial
lowering o~ thè tensile strength`in the 90% polyetherimide

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~27~7~

8CU-3456
- 18 -
blend may be due to the presence of a two phase system.
From the above discussion, it can be observed that
several of the measured properties of the blends reach
a maximum relative to other blends of the total con-
centration range at the 50:50 blend level of polyetherimideto polyamide. Consequently, the concentration range
about the 50:5Q blend level, i.e., from about 40 to
about 60~ polyetherimide is presently preferred for the
~lends of the invention.
Example II
The basic procedure of Example I was repreated using
a nylon 12 sold under the tradename L-2101 by Huls instead
of nylon 6:6. This polyamide along has the properties
set forth at the bottom of Table II. In addition, the
extruder temperature profile varied from about 320 to
32~C for the blends containing 10 and 30% polyetherimide
and from about 315 to 332C for the remainder of the blends.
The die temperature used in preparing all the blends was
about 321.C.
As in Example I, test specimens of each blend were
tested for notched and unnotched Izod impact strength as
~ell as for heat distortion temperature, flexural proper-
ties and tensile properties. These results and the
visual appearance of the various blends are set forth
in Table II.




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8CU-3456
- 20 -

The data from Table II is also plotted in dotted
lines in Figures 1 throu~h 5 versus relative concentra-
tions of the components of the blends. From Figure 1,
a plot of unnotched impact strength values versus
polyetherimide concentration, it is evident that the
unnotched impact decrease from pure polyetherimide
(~6.5 ft-lb/inl to the blend containing 70% polyetherimide
~ontent where the values start to increase and finally
exhibit maximum at approximately 30% polyetherimide.
In a similar manner, the notched Izod impact strength
values of the blends decrease very rapidly between 90%
and 5Q% polyetherimide content and then remain fairly
constant as the concentration of nylon increases further.
The heat distort~on temperature values, plotted
in Figure 2, decrease rapidly from pure polyetherimide
to the 50:50 blend level. Below 50% polyetherimide
the heat distortion temperature values decrease only
slightly as more nylon is included in the blends. This
data suggest a phase inversion occurs around a 50:50
blend composition of the two components.
The flexural strength, plotted in Figure 3, exhibits
behavior similar to the unnotched Izod values where the
values decreases as the polyetherimide concentration is
lo~red to the ~0% level and then increase to a maximum
~5 at approximately a 50:50 blend ratio. The flexural
modulus does not exhibit this same behavior but at the
5Q:50 blend ratio the curve does change slope as is
shown in Figure 4.
The curve formed by the tensile failure strength
in Figure 5 is very similar to both the flexural strength
and Izod curves. A maximum in the tensile failure
strength is found at about a 30% polyetheri~ide com-
position while the tensile failure elongation reaches its
hightest value at 3I%. No tensile yield points are
e~hibited by any o~ these blends.
It is cont`emplated that substitution of other poly-




:, ~ - .

~27~97~
8CU-3456
- 21 -

etherimides and/or other polyamides for the polyetherimides
and/or polyamides in the blends of the above examples
may result in the formulation of polymer blends having
similar characteristics.
While the present invention has been described with
reference to particular embodiments thereof, it will be
~mderstood that numerous modifications may be made by
those skilled in the art withour actually departing from
the spirit and scope of the invention as defined in the
appended claims.

Representative Drawing

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Administrative Status

For a clearer understanding of the status of the application/patent presented on this page, the site Disclaimer , as well as the definitions for Patent , Administrative Status , Maintenance Fee  and Payment History  should be consulted.

Administrative Status

Title Date
Forecasted Issue Date 1990-06-26
(22) Filed 1983-04-22
(45) Issued 1990-06-26
Deemed Expired 1995-12-26

Abandonment History

There is no abandonment history.

Payment History

Fee Type Anniversary Year Due Date Amount Paid Paid Date
Application Fee $0.00 1983-04-22
Registration of a document - section 124 $0.00 1983-06-20
Maintenance Fee - Patent - Old Act 2 1992-06-26 $100.00 1992-03-05
Maintenance Fee - Patent - Old Act 3 1993-06-28 $100.00 1993-04-29
Maintenance Fee - Patent - Old Act 4 1994-06-27 $100.00 1994-05-13
Owners on Record

Note: Records showing the ownership history in alphabetical order.

Current Owners on Record
GILES, HAROLD F., JR.
WHITE, DWAIN M.
GENERAL ELECTRIC COMPANY
Past Owners on Record
None
Past Owners that do not appear in the "Owners on Record" listing will appear in other documentation within the application.
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Document
Description 
Date
(yyyy-mm-dd) 
Number of pages   Size of Image (KB) 
Description 1993-09-22 21 914
Drawings 1993-09-22 5 77
Claims 1993-09-22 8 249
Abstract 1993-09-22 1 26
Cover Page 1993-09-22 1 21
Fees 1994-05-13 1 41
Fees 1993-04-29 1 42
Fees 1992-03-05 1 41