FLAME-RETARDANT, IMPACT-RESISTANT POLYPHENYLENE ETHER COMPOSITIONS

TRADUCTION NON-DISPONIBLE

English Abstract

ABSTRACT OF THE DISCLOSURE
Self-extinguishing thermoplastic molding compositions
having high impact resistance and good surface appearance are
disclosed which comprise, in admixture, (a) a normally flammable
composition comprising a polyphenylene ether resin and a polymer
selected from the group consisting of a hydrogenated A-B-A1
block copolymer and an acrylic resin modified diene rubber
containing resin, and (b) an aromatic phosphate compound in an
amount at least sufficient to render the normally flammable
composition self-extinguishing and, after molding, impact
resistant and having a high surface glass as required for use
in many commercial applications.

Claims

The embodiments of the invention in which an exclu-
sive property or privilege is claimed are defined as follows:
1. A self-extinguishing thermoplastic molding
composition which, after molding, is impact resistant and
has high surface gloss, said composition comprising an intimate
admixture of:
(a) a normally flammable composition comprising
(i) a polyphenylene ether resin, alone, or in combination with
a styrene resin, and (ii) a polymer selected from the group
consisting of a hydrogenated A-B-A1 block copolymer wherein,
prior to hydrogenation, B is a conjugated diene and A and A1
are independently selected from the group comprising homopolymers
and copolymers derived from vinyl aromatic hydrocarbons
and an acrylic resin modified diene rubber-containing resin,
and
(b) an aromatic phosphate compound in an amount
at least sufficient to render said normally flammable
composition (a) self-extinguishing and, after molding, impact
resistant and having a high surface gloss.
2. A self-extinguishing composition as defined
in Claim 1 wherein the polyphenylene ether resin (a) (i) is
of the formula:
<IMG>
wherein the oxygen ether atom of one unit is connected to the
benzene nucleus of the next adjoining unit, n is a positive
integer and is at least 50, and each Q is a monovalent sub-
stituent selected from the group consisting of hydrogen, halogen,
19

hydrocarbon radicals free of a tertiary alpha-carbon
atom, halohydrocarbon radicals having at least two
carbon atoms between the halogen atom and the phenyl
nucleus, hydrocarbonoxy radicals and halohydrocarbonoxy
radicals having at least two carbon atoms between the halogen
atom and thephenyl nucleus.
3. A self-extinguishing composition as
defined in Claim 2 wherein in said polyphenylene ether
resin (a)(i), each Q is alkyl having from 1 to 4 carbon
atoms.
4. A self-extinguishing composition as
defined in Claim 3 wherein in said polyphenylene ether
resin (a)(i), each Q is methyl.
5. A self-extinguishing composition as
defined in Claim 1 wherein the A-B-A1 block copolymer
of component (a)(ii), prior to hydrogenation, is
characterized as follows:
(1) each A is a polymerized mono alkenyl
aromatic hydrocarbon block having an average molecular
weight of about 4,000 to 115,000;
(2) B is a polymerized butadiene hydrocarbon
block having an average molecular weight of about 20,000
to 450,000;
(3) the blocks A constituting 2 to 33 weight
percent of the copolymer;
(4) 35 to 55% of the butadiene carbon atoms
in block B being vinyl side chains;

(5) and the unsaturation of block B having
been reduced to less than 10% of the original unsaturation.
6. A self-extinguishing composition as defined
in Claim 5 wherein the A-B-A1 block copolymer of component
(a)(ii), prior to hydrogenation, is characterized as
follows:
(1) each A is a polymerized styrene
block having an average molecular weight of about
8,000 to 60,000;
(2) B is a polymerized butadiene block
having an average molecular weight of about 50,000 to
300,000, 40 to 50% of the butadiene carbon atoms in
the block being vinyl side-chains;
(3) the blocks A comprising 5 to 30% by weight
of the copolymer; the unsaturation of block B having
been reduced by hydrogenation to less than 10% of its
original value.
7. A self-extinguishing composition as
defined in Claim 1 wherein the acrylic resin modified diene
rubber resin component (a)(ii) is selected from the
group consisting of a resinous composition consisting
essentially of a poly(alkyl-methacrylate) grafted onto a
butadiene-styrene backbone or an acrylonitrile-
butadiene-styrene backbone or a resinous composition
consisting essentially of a mixture of a poly-
(alkylmethacrylate) and a butadiene styrene copolymer
or an acrylonitrile-butadiene-styrene terpolymer, component
(a)(ii) being present in an amount of from about 10
to about 80% by weight of the total resinous components
of the composition.
21

8. A self-extinguishing composition as defined in
Claim 1 wherein the aromatic phosphate flame retarding agent
(b) is of the formula:
<IMG>
wherein R1, R2 and R3 are the same or different, and are alkyl,
cycloalkyl, aryl, alkyl substituted aryl, halogen substituted
aryl, aryl substituted alkyl, halogen, hydrogen and combinations
of any of the foregoing, provided that at least one of R1, R2
and R3 is aryl.
9. A self-extinguishing composition as defined in
Claim 8 wherein said aromatic phosphate is triphenyl phosphate.
10. A self-extinguishing composition as defined in
Claim 1 which includes a reinforcing amount of a fibrous glass
reinforcing filler.
11. A self-extinguishing thermoplastic molding
composition which, after molding, is impact resistant and has
high surface gloss, said composition comprising an admixture of:
(a) a normally flammable composition comprising
(i) a polyphenylene ether resin, alone, or in combination with
a styrene resin, and (ii) a hydrogenated A-B-A1 block copolymer
wherein, prior to hydrogenation, B is a conjugated diene and
A and A1 are independently selected from the group comprising
homopolymers and copolymers derived from vinyl aromatic hydro-
carbons, and
(b) an aromatic phosphate flame retarding
agent in an amount at least sufficient to render said normally
flammable composition (a) self-extinguishing and, after molding,
impact resistant and having a high surface gloss.
22

12. A composition as defined in claim 11 wherein
the polyphenylene ether resin (a)(i) is of the formula:
<IMG>
wherein the oxygen ether atom of one unit is connected to the
benzene nucleus of the next adjoining unit, n is a positive
integer and is at least 50, and each Q is a monovalent substituent
selected from the group consisting of hydrogen, halogen, hydro-
carbon radicals free of a tertiary alpha-carbon atom, halo-
hydrocarbon radicals having at least two carbon atoms between
the halogen atom and the phenyl nucleus, hydrocarbonoxy radicals
and halohydrocarbonoxy radicals having at least two carbon atoms
between the halogen atom and phenyl nucleus.
13. A composition as defined in claim 12 wherein in
said polyphenylene ether resin (a)(i), each Q is alkyl having
from 1 to 4 carbon atoms.
14. A composition as defined in claim 13 wherein
said polyphenylene ether resin (a)(i), each Q is methyl.
15. A composition as defined in claim 11 wherein
the A-B-A1 block copolymer (a)(ii), prior to hydrogenation, is
characterized as follows:
(1) each A is a polymerized mono alkenyl aromatic
hydrocarbon block having an average molecular weight of about
4,000 to 115,000;
(2) B is a polymerized butadiene hydrocarbon block
having an average molecular weight of about 20,000 to 450,000;
(3) the blocks A constituting 2 to 33 weight percent
of the copolymer;
(4) 35 to 55% of the butadiene carbon atoms in
23

block B being vinyl side chains;
(5) and the unsaturation of block B having been
reduced to less than 10% of the original unsaturation.
16. A composition as defined in claim 11 wherein
the A-B-A1 block copolymer (a)(ii), prior to hydrogenation, is
characterized as follows:
(1) each A is a polymerized styrene block having
an average molecular weight of about 8,000 to 60,000;
(2) B is a polymerized butadiene block having an
average molecular weight of about 50,000 to 300,000, 40 to 50%
of the butadiene carbon atoms in the block being vinyl side chains;
(3) the blocks A comprising 5 to 30% by weight of
the copolymer; the unsaturation of block B having been reduced
by hydrogenation to less than 10% of its original value.
17. A composition as defined in claim 11 wherein
the aromatic phosphate flame retarding agent (b) is of the formula:
<IMG>
wherein R1, R2 and R3 are the same or different, and are alkyl,
cycloalkyl, aryl, alkyl substituted aryl, halogen substituted
aryl, aryl substituted alky , halogen, hydrogen and combinations
of any of the foregoing, provided that at least one of R1, R2
and R3 is aryl.
18. A composition as defined in claim 17 wherein
said aromatic phosphate is triphenyl phosphate.
19. A composition as defined in claim 11 which
includes a reinforcing amount of a fibrous glass reinforcing
filler.
20. A self-extinguishing thermoplastic molding
composition which, after molding, is impact resistant and has
high surface gloss, said composition comprising an admixture of:
24

(a) a normally flammable composition comprising
(i) a polyphenylene ether resin, alone, or in combination with
a styrene resin, and (ii) an acrylic resin modified diene rubber-
containing resin, and
(b) an aromatic phosphate flame retarding agent in an
amount at least sufficient to render the normally flammable
composition (a) self-extinguishing and, after molding, impact
resistant and having a high surface gloss.
21. A composition as defined in claim 20 wherein
the polyphenylene ether resin (a)(i) is of the formula:
<IMG>
wherein the oxygen ether atom of one unit is connected to
the benzene nucleus of the next adjoining unit, n is a positive
integer and is at least 50, and each Q is a monovalent substituent
selected from the group consisting of hydrogen, halogen, hydro-
carbon radicals free of a tertiary alpha-carbon atom, halo-
hydrocarbon radicals having at least two carbon atoms between
the halogen atom and the phenyl nucleus, hydrocarbonoxy radicals
and halohydrocarbonoxy radicals having at least two carbon atoms
between the halogen atom and the phenyl nucleus.
22. A composition as defined in claim 21 wherein in
said polyphenylene ether resin (a)(i), each Q is alkyl having
from 1 to 4 carbon atoms.
23. A composition as defined in claim 22 wherein
in said polyphenylene ether resin (a)(i), each Q is methyl.

24. A self-extinguishing composition as defined in
claim 20 wherein the acrylic resin modified diene rubber resin
component (a)(ii) is selected from the group consisting of a
resinous composition consisting essentially of a poly(alkyl-
methacrylate) grafted onto a butadiene-styrene backbone or an
acrylonitrile-butadiene-styrene backbone or a resinous composition
consisting essentially of a mixture of a poly(alkylmethacrylate)
and a butadiene styrene copolymer or an acrylonitrile-butadiene-
styrene terpolymer, component (a)(ii) being present in an amount
of from about 10 to about 80% by weight of the total resinous
components of the composition.
25. A composition as defined in claim 20 wherein the
aromatic phosphate flame retarding agent (b) is of the formula:
<IMG>
wherein R1, R2 and R3 are the same or different, and are alkyl,
cycloalkyl, aryl, alkyl substituted aryl, aryl substituted alkyl,
halogen, hydrogen and combinations of any of the foregoing, pro-
vided that at least one of R1, R2 and R3 is aryl.
26. A composition as defined in claim 25 wherein
said aromatic phosphate is triphenyl phosphate.
27. A composition as defined in claim 20 which includes
a reinforcing amount of a fibrous glass reinforcing filler.
26

Description

~ 32 8CH-2146
This invention relates to novel thermoplastic
molding compositions which are self-extinguishing and are
moldable to finished articles of good impact resistance and
high surface gloss. More particularly, the invention i5
concerned with thermoplastic compositions of a polypheny-
lene ether resin, a polymer selected from hydrogenated
A-B-A block copolymers and acrylic resin modified diene
rubber containing resins, and an aromatic phosphate which
is present in amounts sufficient to provide, in addition
to flame resistance to the thermoplastic impurities, impact
resistance and good surface gloss to the resulting molded
articles.
The polyphenylene ether resins are well known in
the art as a class of thermoplastics which possess a
number of outstanding physical properties. They can be
prepared by oxidative and non-oxidative methods, such as are
disclosed, for example, in Hay, U.S. Patent 3,306,874 dated
February 28, 1967 and 3,306,875 dated February 28, 1967 and
Stamatoff, U.S. Patent 3,257,357 dated June 21, 1966 and
3,257,358 dated June 21, 1966.
It has been found that many of the properties
of polyphenylene ether resins, e.g., ease of processing,
impact strength and solvent resistance, can be improved by
combining these resins with other resins, such as, for
example, polystyrene. Examples of polyphenylene ether
resin-polystyrene compositions are disclosed in Cizek, U.S.
Patent 3,383,435 dated May 14, 1968.
More recently, it has been found that polypheny-
lene ether resins can also be combined with block copolymers
of the A-B-A type, e.g., polystyrene-polybutadiene-poly-
styrene, and with acrylic resin modified diene rubber
containing resins, to provide compatible compositions
~k

~2~32 8CH-2146
characterized by a number o~ excellent physical properties
in the resulting molded articles. These discoveries are
described in Abolins et al, U.S. 3,833,688 dated September
3, 1974 and 3,792,123 dated February 12, 1974 and in
Canadian application Serial No. 205,298, filed July 22,
1974, and assigned to the same assignee as in the present
application.
It is known in the art that the polyphenylene
ethers have excellent flame retardant properties and are
classified self-extinguishing and non-dripping according
to ASTM Test Method D635 and Underwriters Laboratories
Bulletin No. 94. On the other hand, when polyphenylene
ethers are combined with other polymers such as the above-
mentioned A-B-A block copolymers and acrylic resin modified
diene rubber containing resins, many of the resulting com-
positions have poor flame retardancy and are not self-
extinguishing, but rather burn slowly upon ignition. Con-
sequently, many compositions of polyphenylene ether resin
and A-B-Al block copolymers or acrylic resin modified diene
rubber containing resins are unable to meet the minimum
requirements established by various testing laboratories
such as the Underwriters Laboratories. This restricts the
use of such compositions for many commercial applications.
Flame retardant additives for thermoplastics are
known. In general, these are either blended physically with
the thermoplastic or are used to unite chemically with the
plastic and to modify it. For instance, self-extinguishing
blends of a polyphenylene ether resin and a styrene resin
using a combination of an aromatic phosphate and an aromatic
halogen for flame retardancy are disclosed by Haaf in U.S.
3,639,506 dated February 1, 1972. Other self-extinguishing
polyphenylene ether-polystyrene compositions are disclosed

11~2~3z 8CH-2146
by Reinhard in U.S. 3,809,72g, dated May 7, 1974 wherein
aromatic halogens combined with antimony compounds are used
as flame retardant additives. Still other flame retardant
compositions of a polyphenylene ether resin and a styrene
resin which include various phosphorus-containing and
halogen-containing flame retardant agents, are described by
Haaf et al in Canadian Serial No. 242,338 filed December 18,
1975 and assigned to the same assignee as herein.
However, as is also well known, the inclusion of
flame retarding compounds in thermoplastic materials not only
affects burning characteristics, it frequently changes other
physical properties as well, such as color, flexibility,
tensile strength, electrical properties, softening point, and
moldability characteristics. Thus, for example, aromatic
phosphates such as triphenyl phosphate have been added to
blends of polyphenylene ethers and styrene resins, with
flame retardant properties being improved to the point where
the compositions can be classified as self-extinguishing and
non-dripping according to the above-noted ASTM Test Method
D635 and U.L. Bulletin No. 94.
It has now been surprisingly discovered that
molded compositions consisting of polyphenylene ether or
various combinations of polyphenylene ether and polystyrene,
certain polymeric modifiers, and aromatic phosphate com-
pounds exhibit excellent self-extinguishing behavior,
impact strength and surface gloss.
The commercial benefits of flame retardancy, good
impact resistance and high surface gloss in the composition
of this invention are most unexpected, generally in view of
the physical properties frequently exhibited by flame
retardant compositions of the prior art.
Description of the Invention - According to

' 8c~-2146
2~32
I
1 ¦ the present invention there are provided flame retardant
2 ¦ self-extinguishing thermoplastic molding compositions which,
3 ¦ after molding, are impact resistant and have high surface gloss,
4 ¦ the compositions comprising an intimate admixture of:
¦ (a) a normally flammable compositi~n
6 ¦ comprising (i) a polyphenylene ether resin and (ii) a polymer
7 selected from the group consisting of a hydrogenated A-B-A
block copolymer and an acrylic resin modified diene rubber-
9 containing resin, and "
(b) an aromatic phosphate compound in an
11 amount at least sufficient to render the normally flammable
12 composition self-extinguishing and, after molding, impact
13 resistant and having a high surface gloss.
14 .
The polyphenylene ether resins of (a) are
16 preferably of the type having the structural formula:
17
~1 - 3~
24 wherein the oxygen ether atom of one unit is connected to the
benzene nucleus of the next adjoining unit, n is a positive
26 integer and is at least 50, and each Q is a monovalent
27 substituent selected from the group consisting of hydrogen,
28 halogen, hydrocarbon radicals free of a tertiary alpha-carbon
29 atom, halohydrocarbon radicals having at least two carbon
atoms between the halogen atom and the phenyl nucleus,

1 8CH-2146
1~2~3Z
, .'
1 hydrocarbonoxy radicals and halohydrocarbonoxy radicals having
2 a~ least two carbon atoms between the halogen atom and the
3 phenyl nucleus.
An especially preferred class of polyphenylene
6 ether resins for the compositions of this invention includes
7 those of the above formula wherein each Q is alkyl, most preferab~ Y
8 having from 1 to 4 carbon atoms. -Illustratively, members of this
9 class include poly(2,6-dimethyl-1,4-phenylene)ether; poly
(2,6-diethyl-1,4-phenylene)ether; poly(2-methyl-6-ethyl-1,4-
11 phenylene)ether; poly(2-methyl-6-propyl-1,4-phenylene)ether;
12 poly(2,6-dipropyl-1,4-phenylene)ether; poly(2-ethyl-6-propyl-1,
13 4-phenylene)ether; and the like. Most preferred is poly(2,6-
14 dimethyl-1,4-phenylene)ether, preferably having an intrinsic
viscosity of about 0.45 decililiters per gram (dl./g.) as measured
16 in chloroform at 30C.
17
18 The hydrogenated A-B-Al block copolymers of
19 component (a)(ii) are well known. In general, these are block
copolymers of the A-B-Al type in which terminal blocks A and A
21 are the same or different and, prior to hydrogenation, comprise
22 homopolymers or copolymers derived from vinyl aromatic hydro-
23 carbons and, especially, vinyl aromatics wherein the aromatic
24 moiety can be either monocyclic or polycyclic. Examples of
the monomers are styrene, alpha methyl styrene, vinyl xylene,
26 ethyl vinyl xylene, vinyl naphthalene, and the like. Center
block B will always be derived from a conjugated diene, e.g.,
29 butadiene, isoprene, 1,3-pentadiene, and the like. Preferably,
center block B will be comprised of polybutadiene or polyiso-
prene.

j~ 8CH- 2146
~2(;~32
1 . .
2 It is preferred to form t:erminal blocks A and A
having average molecular weights of 4,000 to 115,000 and center
4 block B having average molecular weights of 20,000 to 450,000.
Still more preferably, the terminal blocks will have average
molecular weights of 8,000 to 60,000 while the center block
76 has an average molecular weight between about 50,000 and .,
8 300,000. The terminal blocks will preferably comprise from 2 to Il.
9 33% by weight, and more preferably, 5 to 30% by weight of the
total block copolymer. Especially preferred are A-B-Al type
11 block copolymers having apolybutadiene center block wherein
12 35 to 55%, or more preferably, 40 to 50% of the carbon atoms
13 present in the butadiene polymer block are in the form of
154 dependent vinyl side chains.
16 The A-B-Al block copolymers will have an
17 unsaturation in the center block B reduced to less than 10%
18 and more preferably, less than 5% of its original value.
The hydrogenated block copolymers are formed
21 by techniques which are well known to those skilled in the art.
22 For instance, the preparation of these materials is described
23 in detail in Jones, U.S. 3,431,323, dated March 4,
24 1969.
26 Hydrogenation can be carried out with a variety
27 of ~ydrogenation catalysts, such as nickel on Kieselguhr, Raney
28 nickel, copper chromate, molybdenum sulfide and finely divided
29 platinum or other noble metals on a low surface area catalyst.
Hydrogenation can be conducted at any desired

il 8CH- 2146
Q3Z
1 te~ ~erat~re or press~rè, e g , from anmospheric t~ 3,0~0 p.9.i.g.,
2 the usual ange being between 100 and 1,000 p.s.i.g., and at tem-
3 ~ peratures from about 75 to 600F., for times between 0.1 and 24
4 hours, preferably 0.2 to 8 hours.
The acrylic resin modified diene rubber resin of com-
6 ponent (a)(ii) i9 preferably selected from the group consisting
7 o a resinous composition consisting essentially of a poly(alkyl-
8 methacrylate) grafted onto a butadiene-styrene backbone or an
9 acrylonitrile-butadiene-styrene backbone or a resinous composition
consisting essentially of a mixture of a poly(alkylmethacrylate)
11 and a butadiene styrene copolymer or an acrylonitrile-butadiene-
12 styrene terpolymer.
13 The graft polymerization product of an acrylic monomer
14 and a diene rubber of component (a)(ii) preferably comprises (1)
from about 20 to 80% by weight of a backbone copolymer of butadien~
16 and styrene or a backbone terpolymer of acrylonitrile, butadiene
17 and styrene, wherein the butadiene units are present in quantities
18 of at least 40% by weight of the backbone polymer; (2) 80 to 20%
19 by weight of an acrylic monomer graft polymerized to (1), said
acrylic monomer units being selected from the group consisting of
21 lower alkyl methacrylates, alicyclic methacrylates and alkyl
22 acrylates, and (3) 0 to 60% by weight of a styrene monomer graft
23 polymerized to (1).
24 The graft polymerization product of an acrylic
monomer alone or with styrene monomer and the rubbery diene
26 polymer or copolymer may be prepared by known techniques,
27 typically by emulsion polymerization. They may be formed from
28 a styrene-butadiene copolymer latex and a monomeric material
29

8CH-2146
~ 32
such as methyl methacrylate alone or with another compound
having a single vinylidene group copolymerizable therewith,
e.g., styrene. For example, in the preparation of a repre-
sentative material, 85 to 65 parts by weight of monomeric
methyl methacrylate or monomeric methyl methacrylate to the
extent of at least 55%, and preferably as much as 75~ by
weight, in admixture with another monomer which copolymerizes
therewith, such as ethyl acrylate, acrylonitrile, vinylidene
chloride, styrene, and similar unsaturated compounds containing
a single vinylidene group, is added to 15 to 35 parts by weight
of solids in a styrene-butadiene copolymer latex. The copolymer
solids in the latex comprise about 10 to 50% by weight of styrene
and about 90 to 50~ by weight of butadine and the molecular
weight thereof is within the range of about 25,000 to 1,500,000.
The copolymer latex of solids in water contains a dispersing
agent, such as sodium oleate or the like, to maintain the
copolymer in emulsion. Interpolymerization of the monomer or
monomeric mixture with the copolymer solids emulsified in
water is brought about in the presence of a free-radical
generating catalyst and a polymerization regulator which serves
as a chain transfer agent, at a temperature in the range between
15C. and 80C. Coagulation of the interpolymerized product
is then effected with a calcium chloride solution, for instance,
whereupon it is filtered, washed and dried.
Other graft copolymers which differ from the
above only in the ratio of monomeric material comprised solely
or preponderantly of methyl methacrylate to the butadiene
styrene copolymer latex extend from 85 to 25 parts by weight
of the former to 15 to 75 parts by weight of the latter. These
-- 8 --

8C~-2146
1~32~3Z
materials can vary in physical properties from relatively rigid
compositions to rubbery compositions. A preferred commercially
available material is Acryloid KM 611TM, which is sold by
Rohm & Haas Company. Additional information on the preparation
of these materials is contained in U.S. 2,943,074 dated June 28,
1960 and in U.S. 2,857,360 dated october 21, 1958. A preferred
material is described in U.S. 2,943,074, Column 4, preparation
"D" with conversion to emulsified polymer "B" described therein.
The aromatic phosphate compound of the
compositions of the invention is a compound of the formula:
R30 - P ORl
l R2
where Rl, R2 and R3 can be the same or different and are alkyl,
cycloalkyl, aryl, alkyl substituted aryl, halogen substituted aryl,
aryl substituted alkyl, halogen, hydrogen and combinations of any
of the foregoing, provided that at least one of Rl, R2 and R3 is
aryl.
Typical examples include phenylbisdodecyl
phosphate, phenylbisneopentyl phosphate, phenylethylene hydrogen
phosphate, phenyl-bis(3,5,5'-trimethylhextyl phosphate), ethyl-
diphenyl phosphate, 2-ethyl-hexyldi(p-tolyl) phosphate, di-phenyl
hydrogen phosphate, bis (2-ethylhexyl) p-tolylphosphate, tri-
tolyl phosphate, bis (2-ethylhexyl)phenyl phosphate, tri-(nonyl-
phenyl) phosphate, phenylmethyl hydrogen phosphate, di(dodecyl)
p-tolyl phosphate, tricresyl phosphate, triphenyl phosphate,
dibutylphenyl phosphate, 2-chloroethyldiphenyl phosphate,

8CH-2146
~2~32
p-tolyl bis (2,5,5'-trimethylhexyl) phosphate, 2-ethylhexyl-
diphenyl phosphate, diphenyl hydrogen phosphate, and the like.
The preferred phosphates are those where each R is aryl.
Especially preferred is triphenyl phosphate.
The respective amounts of the components in the
present compositions can vary broadly, e.g., from 60 to 99
parts by weight of polyphenylene ether resin to 40 to 1 parts
by weight of A-s-Al block copolymer or acrylic resin modified
diene rubber containing resin. With respect to the compositions
containing A-B-Al block copolymers, the most preferred such
compositions contain no less than about 65% by weight of poly-
phenylene ether alone or combined with polystyrene resin, based
on the total weight of the resinous components in the composi-
tion. With respect to the aromatic phosphate flame retarding
agent, amounts of from 1 to 40 parts by weight of the total
composition can be employed to impart flame retardancy. Par-
ticular amounts will, of course, vary depending on the needs
of the specific composition.
The compositions of the invention can also further
include glass fibers as a reinforcing filler, especially pre-
ferably, fibrous glass filaments comprised of line-aluminum
borosilicate glass which is relatively soda free, known as "E"
glass. However, other glasses are useful where electrical prop-
erties are not so important, e.g., the low soda glass known as
"C" glass. The filaments are made by standard processes, e.g., by
steam or air blowing, flame blowing and mechanical pulling. The
preferred filaments for plastics reinforcement are made by
mechanical pulling. The filament diameters range from about
-- 10 --

8CH-2146
32
0.000112 to 0.00075 inch, but this is not critical to the
present invention.
In general, best properties will be obtained if
the sized filamentous glass reinforcement comprise from about
1 to about 80% by weight based on the combined weight of glass
and polymers and preferably, from about 10 to about 50% by
weight. Especially preferably, the glass will comprise from
about 10 to about 40% by weight based on the combined weight
of glass and resin. Generally, for direct molding use, up to
about 50% of glass can be present without causing flow problems.
However, it is useful also to prepare the compositions con-
taining substantially greater quantities, e.g., up to 70 to 80%
by weight of glass. These concentrates can then be custom
blended with blends of resins that are not glass reinforced
to provide any desired glass content of a lower value.
Other ingredients, such as stabilizers, pigments,
plasticizers, antioxidants, and the like, can be added for their
conventionally employed purposes.
The compositions of this invention can be prepared
conventionally by tumbling the components to form a preblend,
extruding blend into a continuous strand, cutting the strand
into pellets or granules, and molding the pellets or granules
into the desired shape. These techniques are well known to
those skilled in the art and further elaboration herein is not
necessary.
Description of the Preferred Embodiments. - The

- ¦¦ 8CH-2146
~02(~3;~
1 following examples illustrate compositions according to the
2 invention. They are set forth for illustrative purposes only,
3 and are not to be construed as limit:ing.
EXAMPLES 1 - 10
6 The compositions shown in Table I, below, were
7 prepared by preblending the components, extruding the blend
8 and molding the extrudate into test pieces. All amounts
are in parts by weight. The values for Izod impact strength
are in units of ft.lbs./in.n., and the values for Gardner
11 impact strength are in units of in.-lbs. Tensile yield,
12 tensile break, flexural yield and flexural modulus values
13 are each in units of p.s.i. x 10-3. The gloss values are 45
surfac loss expressed as relative dimensionless units.
22
29 '~
_ _ - 12 -
::: ..... .

~ 2~32 ~
8CH--2146
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.,
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2~32
ll 8CH-2146
I EXAI~LES 11 - 18
2 Additional compositions according to the
3 invention were prepared and tested as in Examples l to lO.
4 The formulations and test results for the additional
composition.s are listed in Table II. Unless shown otherwise,
1~ units a as in T~b1e I.
~4
18
23
24
26
239
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~Z~32 8CH--2146
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~Z~32 8CH-2146
Although the above examples illustrate various
modifications of the present invention, other variations
will suggest themselves to those skilled in the art in the
light of the above disclosure. It is to be understood,
therefore, that changes may be made in the particular
embodiments described above which are within the full intended
scope of theinvention as defined in the appended claims.
The instant appllcation discloses and claims subject
matter disclosed but not claimed in the related, commonly
assigned Canadian Application Serial No. 292,795, filed December
9, 1977.
- 18 -