Note: Descriptions are shown in the official language in which they were submitted.
2184778
STYRENE-BASED RESIN COMPOSITION
FTT'T n OF T~IE T~VET\TTION
The present invention relates to a syndiotactic,
polystyrenic resin composition. More precisely, it relates
to a syndiotactic, polystyrenic resin composition which can
be formed into an article having improved heat resistance,
an increased modulus of elasticity and greatly improved
toughness, and in addition, the peeling of the surface layer
of the article to be formed from the composition is
retarded.
R~t~K~TROUND OF TF~ TNVFI\TTI~
Articles formed from a styrene-based polymer having a
syndiotactic configuration (hereinafter referred to as SPS)
have excellent heat resistance and chemical resistance but
have poor impact resistance. Therefore, the polymer has
heretofore been used in limited ranges. In order to improve
the impact resistance of SPS articles, it has been proposed
to add rubber-like elastic substances and other
thermoplastic resins to SPS (see Japanese Patent Application
Laid-Open Nos. 257950/1987, 146944/1989, 182344/1989,
279944/1989, and 64140/1990).
Concretely, a composition comprising SPS and, as a
rubber-like elastic material, a component containing a
styrenic compound (see Japanese Patent Application Laid-Open
2184778
No. 146944/1989), and a composition comprising a mixture of
SPS and a thermoplastic resir and/or a rubber-like polymer
except SPS, and, as a miscibility-improving agent, a
styrenic chain-containing, block or graft copolymer ~see
Japanese Patent Application ~aid-Open No. 279944/1989) have
been proposed.
These compositions contain, as a miscibility-improving
agent, a polystyrenic chain-containing, block or graft
polymer, in order to improve the miscibility of a rubber
component with immiscible SPS and to improve the
dispersibility of the rubber component and the interfacial
strength between the constitutive components However, the
effect of the miscibility-improving agent therein is not
satisfactory. ~herefore, the articles formed from these
compositions are not q~ti cf~-torily tough and the peeling of
the surface layers from the articles could not be retarded
suf ficiently .
STTMM~Ry OF ~ I~VF~rIoN
Given the situations, it is an obj ect of the present
invention to provide a syndiotactic, polystyrenic resin
composition which can be formed into an article having an
increased modulus of elasticity, high heat resistance and
greatly improved toughness, and additionally having high
impact resistance while retarding the peeling of the surface
layer from the article.
~ 21~778
We, the inventors o~ the present invention have
assiduously studied so as to develop a syndiotactic,
polystyrenic resin composition having the above-mentioned
favor_ble properties and, as a result, have found that the
intended object can be attained by a composition comprising
a styrene-based polymer having a syndiotactic configuration
and a polyolefin and, as a miscibility-improving agent for
these, a particular styrene-olefin copolymer, in
pr,~ t~rm;ned ratios. ~n addition, we have found that, when
a small amount of a polyp~enylene ether is added to the
composition, the toughness of an article to be formed from
the resulting composition can be more effectively improved.
Moreover, we have further ~ound that, when a particular
styrene-based copolymer and/or a particular oil or wax
are/is added thereto, the toughness of the article can be
much more effectively improved. Furthermore, we have found
that, when an inorganic filler, or a combination of an
inorganic f iller and a particular polymer having a polar
group is added to the composition in predetermined ratios,
the heat resistance and the modulus of elasticity of the
article can be much more increased. On the basis of these
f indings, we have completed t~e present invention .
SP"t';~;~A11Y, the present invention provides;
(1) a syndiotactic, polystyrenic resin composition
comprising resin components of (A) 100 parts by weight of a
1- 218~778
component composed of (a) from 10 to 98 96 by weight of a
styrene-based polymer having a syndiotactic configuration
and (b) from 2 to 90 % by weight of a polyolefin, and (B)
from 0.5 to 50 parts by weight of a styrene-olefin copolymer
having a styrene content of from 40 to 85 9~ by weight;
(2) a syndiotacticl polystyrenic resin composition
comprising resin components of (A) 100 parts by weight of a
component composed of (a) from 10 to 98 % by weight of a
styrene-based polymer havinç~ a syndiotactic configuration
and (b) from 2 to 90 9~ by weight of a polyolefin, (~) from
0 . 5 to 50 parts by weight of a styrene-olefin copolymer
having a styrene content of from 40 to 85 96 by weight, and
(C) from 0.5 to 10.0 parts by weight, relative to 100 parts
by weight of the component-ZaT of (A), of a polyphenylene
ether (having an intrinsic ~iscosity in chloroform at 25 C
of 0 . 4 dl/g or higher);
(3 ) a syndiotactic, polystyrenic resin composition of
the above-mentioned (1) or (2), which further contains (D)
from 0 to 200 parts by weight, relative to 100 parts by
weight of the component (~) of (A), of a styrene-olefin
copolymer having a styrene content of from 5 to 35 96 by
weight; ~ ~
(4) a syndiotactic, pol~styrenic resin composition of
the above-mentioned (1) or~r2~, which further contains (E)
from 0 to 200 parts by we~ght, relative to 100 parts by
2184778
1~
weight of the component (b) of (A), of a paraffinic oil, a
paraffinic waY, a mineral oil and/or a siloxanic oil; and
(5) a syndiotactic, polystyrenic resin composition of
the sbove-mentioned (1) or (2), which further contains (D)
from 0 to 200 parts by weight, relative to 100 parts by
weight of the component i(b) of (A), of a styrene-olefin
copolymer having a styrene content of from 5 to 35 % by
weight, and (E) from 0 to 2~0 parts by weight, relative to
100 parts by weight of the. component (b) of (A), of a
paraffinic oil, a paraffinic waY, a mineral oil and/or a
s; l ~Y~n; C oil .
Preferred embodiments of the present invention are;
(6) the syndiotactic, polystyrenic resin composition of
any of the above-mentioned (1) to (5), which further
contains (F) from 0 . 5 to 350 parts by weight, relative to
100 parts by weight of the resin components, of an inorganic
f iller, and
(7) the syndiotactic, polystyrenic resin composition of
any of the above-mentioned (1) to (5), which further
contains (E) from 0 . 5 to 350 parts by weight, relative to
100 parts by weight of the resin components, of an inorganic
filler, and (G) from 0.1 to 10 parts by weight, relative to
the same, of a polymer which is miscible with or has an
affinity for the component (a) of (A) and which has a polar
group .
2~847~8
DE~ATT~T~n nT~Cl?TPTION OF TETT' J~VE~TION
The resin composition of the present invention
comprises, as the component (a) of (A), a styrene-based
polymer having a syndiotactic conf iguration . The
syndiotactic configuration irr= the styrene-based polymer as
referred to herein indic~tes that the stereochemical
structure of the polymer is sy~diotactic or, that is, such
that the phenyl groups or substituted phenyl groups which
are in the side chains of the polymer are located
alternately in opposite directions relative to the main
chain of the polymer that c~sists of carbon-carbon bonds.
The tacticity of the polymer is s~uantitatively determined
through nuclear magnetic resonance thereof using a carbon
isotope (13C-NMR). The tacticity as (1~ti~n;n~1 through 13C-
NMR can be represented by the proportions of the structural
units as continuously connected to each other, for example,
in terms of diad for two structural units, triad for three
structural units and pentad ~or five structural units. The
styrene-based polymer having a syndiotactic coniguration as
referred to herein ;nc~ e=~ for example, polystyrene,
poly (alkylstyrene), poly (halogenostyrene),
poly ( halogenoalkyl s tyrene ), poly ( alkoxys tyrene ), poly (vinyl
benzoate), hydrogenated polymers of these, mixtures o~
these, and copolymers consisting essentially of these, which
have generally 75 % or more, preferably 85 96 or more of
2184778
syndiotacticity of racemic diad, or have generAlly 30 96 or
more, preferably 50 9~ or more of syndiotacticity of racemic
pentad. The poly(alkylstyrene) includes, for example,
poly(methylstyrene), poly(ethylstyrene),
poly ( isopropylstyrene), poly ( tert-butylstyrene),
poly(phenylstyrene), poly(vinylnaphthalene), and
poly(vinylstyrene). The poly(halogenostyrene) includes, for
example, poly(chlorostyrene), poly(bromostyrene), and
poly(fluorostyrene) . The poly(halogenoalkylstyrene)
includes, for example, poly(chloromethylstyrene). The
poly(alkoxystyrene) includes, for example,
poly (methoxystyrene), and poly (ethoxystyrene) .
Of these styrene-based polymers, especially preferred
are polystyrene, poly(p-methylstyrene), poly(m-
methylstyrene), poly (p-tert-butylstyrene), poly (p-
chlorostyrene), poly(m-chlorostyrene), poly(p-
fluorostyrene), hydrogenated polystyrene, and copolymers
comprising structural units of these.
The molecular weight of the styrene-based polymer for
use in the present invention is not specifically defined.
Preferably, however, the polymer has a weight average
molecular weight of 10,000 or more, more preferably 50,000
or more. The molecular weight distribution of the polymers
is not also defined. Various polymers having different
molecular weights can be applied to the present invention.
2184778
.
However, polymers having a weight average molecular weight
of less than 10, 000 are undesirable, since the thermal and
mechanical properties of the composition, if comprising any
of such polymers, and those of the articles to be formed
from the composition often tend to be poor.
The styrene-based polymer having a syndiotactic
configuration for use in the present invention can be
obtained, for example, by polymerizing a styrenic monomer
(capable of giving any of the above-mentioned styrene-based
polymers) in the presence of a catalyst composed of titanium
compound and a condensate to be produced from wa~er and a
trialkyl aluminium, in an inert hydrocarbon solvent or in
the absence of such a solvent ( see Japanese Patent
Application Laid-Open No. 187708/1987) .
Poly (halogenoalkylstyrene) s capable of being employed in the
present invention can be obtained, for example, according to
the method described in Japanese Patent Application ~aid-
Open No. 46912/89; and hydrogenated polymers for use in the
invention can be obtained, for example, according to the
method described in Japanese Patent Application Laid-Open
No. 17850~/89.
The styrene-based polymers having a syndiotactic
configuration, which shall constitute the component (a) of
(A) in the composition of the present invention, can be used
either sin~ly or as combined.
21~7~
.
The component (b) of (A) in the composition of the
invention is a polyolefin, which may comprise monomer units
to be derived from any of olefins and dienes such as
ethylene, propylene, butylene, butene, octene, butadiene,
isoprene, norbornene, norbornadiene, and cyclopentadiene.
It ;n~ any known polyolefins. Specific examples of the
polyolefin are ethylene-propylene copolymer rubber (EPM),
ethylene-propylene-diene copolymer rubber (EPDM), isotactic
polypropylene, syndiotactic polypropylene, atactic
polypropylene, block polypropylene, random polypropylene,
high-density polyethylene, high-pressure-process, low-
density polyethylene, linear, low-density polyethylene,
cyclic polyolefins, and copolymers to be obtained from two
or more monomers constituting these polymers. Of these,
preferred are EPM, EPDM, polypropylene and polyethylene.
The polyolefins that shall constitute the component (b)
can be used either singly or as combined.
In the composition of the present invention, the
component (A) comprises from 10 to 98 % by weight,
preferably from 20 to 95 % by weight, more preferably from
30 to 90 % by wei~ht of the above-mentioned component (a),
and from 2 to 90 % by weight, preferably from 5 to 80 ~6 by
weight, more preferably from 10 to ~0 % by weight of the
above-mentioned component (b). If the amount of the
component (a) of (A) is less than the above-mentioned range,
218~778
.
the composition will lose the characteristics of the
syndiotactic polystyrene, and the modulus of elasticity and
the heat resistance of the article to be formed from the
composition will be noticeahly lowered. If, on the other
hand, it is more than the range, the toughness of the
article could not be satisfactorily improved.
The composition of the present invention comprises from
0.5 to 50 parts by weight, relative to 100 parts by weight
of the component (A), of the component (B) which is a
styrene-olefin copolymer having a styrene content of from 40
to 85 96 by weight. The component (B) acts as a miscibility-
improving agent for the components (a) and (b) that
constitute the component (A). The block copolymer of the
component (B) must have a styrene content of from 40 to 85 9s
by weight. Preferably, the copolymer has a melt viscosity
of 1200 Pa-sec or less at a temperature of 300 C and at a
shearing rate of 100 sec~l.
If the styrene content cf the copolymer is outside the
defined range, the copolymer of the component (B) could not
sufficiently function as a mlscibility-improving agent for
the components (a) and (b). If so, the toughness of the
article to be formed from the composition is low, the
peeling of the surface layer from the article could not be
satisfactorily retarded, and therefore the objects of the
present invention could not~be attained satisfactorily. In
; 218~778
view of its miscibility-improving function, the styrene
content of the copolymer of the component (B) is preferably
from 45 to 80 96 by weight, more preferably from 50 to 75 %
by weight. If, on the other hand, the melt viscosity of the
copolymer (this is a parameter of the molecular weight of
the copolymer) is more than 1200 Pa-sec, the copolymer could
not sufficiently function as a miscibility-improving agent
for the components (a) and (b) and, as a result, the objects
of the present invention could not be ~tti3;nPll~
The styrene-olefin copolymer of the component (B)
includes, for example, styrene-butadiene random copo~ymer,
hydrogenated styrene-butadiene random copolymer, styrene-
isoprene random copolymer, hydrogenated styrene-isoprene
random copolymer, styrene-butadiene block copolymer (SBR),
hydrogenated styrene-butadiene block copolymer (SEB, SEBC),
styrene-butadiene-styrene block copolymer (SBS),
hydrogenated styrene-butadiene-styrene block copolymer
(SEBS), styrene-isoprene block copolymer (SIR), hydrogenated
styrene-isoprene block copolymer (SEP), styrene-isoprene-
styrene block copolymer (SIS), hydrogenated styrene-
isoprene-styrene block copolymer (SEP~), styrene-et~ylene
copolymer, styrene-propylene copolymer, ethylene-styrene
graft copolymer, propylene-styrene graft copolymer, EPM-
styrene graft copolymer, EPDM-styrene graft copolymer, and
their modificate:.. of these, preferred are styrene-olefin
11
218~778
.
diblock copolymers ana styrene-ole~in triblock copolymers,
which include, for example, styrene-butadiene block
copolymer (SEB, SEBC), styrene-butadiene-styrene block
c op o lymer ( SB S ), hydro g ena ted s tyr e n e -bu tad i ene - s tyr ene
block copolymer (SEBS), styrene-isoprene block copolymer
(SIR), hydrogenated styrene-isoprene block copolymer (SEP),
styrene-isoprene-styrene block copolymer (SIS), hydrogenated
styrene-isoprene-styrene block copolymer (SEPS) and their
m<~l; f; f ~tes .
The olefin moiety of the component (B) is preferably
compatible with the component (b) of (A). The component (B)
may comprise one or more such styrene-olefin copolymers.
The composition of the present invention shall comprise
from O . S to 50 parts by weight, relative to 100 parts by
weight of the component (A), of the component (s). If the
content of the component (B) is less than 0.5 parts by
weight, the miscibility-improving effect o the component
(s) is insufficient. If so, therefore, the toughness of the
article to be formed from the composition could not be
improved satisfactorily and the peeling of the surface layer
from the article could not be sufficiently retarded.
However, even if the content is more than 5 0 parts by
weight, any more i~ uV~L~ lt in the toughness of the article
and in the retardation of the peeling of the surface layer
from the article could not be expected. Therefore, if too
12
218~778
much amount of the component (B) over the defined range is
added to the composition of the invention, such is
unfavorable since the cost of the composition is increased.
In view of the toughness and other properties of the article
to be formed from the composition and of the intended object
of retarding the peeling of th~e surface layer from the
article, the content of the component (B) is preferably from
1 to 40 parts by weight, more preferably from 3 to 30 parts
by weight.
If desired, the resin composition of the present
invention may optionally contain, as the third component
(C), a polyphenylene ether. Polyphenylene ethers are known,
for which, for example, referred to are U S. Patents
3, 306, 874, 3, 306, 875, 3, 257, 357 and 3, 257, 358 . Concretely,
homopolymers or copolymers of polyphenylene ethers for use
in the present invention can be produced from one or more
phenolic compounds as substituted at two or three positions
thereof, through oxidative coupling in the presence of a
copper-amine complex. The copper-amine complex to be used
may be derived from primary, secondary and tertiary amines.
Suitable examples of polyphenylene ethers for use in the
present invention include poly(2,3-dimethyl-6-ethyl-1,~-
phenylene ether); poly(2-methyl-6-chloromethyl-1,4-phenylene
ether); poly(2-methyl-6-11y-1rwcy~thyl-1,4-phenylene ether);
poly(2-methyl-6-n-butyl-1,4-phenylene ether); poly(2-ethyl-
13
218~778
6-isopropyl-1,4-phenylene ether); poly(2-ethyl-6-n-propyl-
1, 4-phenylene ether); poly(2, 3, 6-trimethyl-1, 4-phenylene
ether); poly[2- (4 ' -methylphenyl) -1, 4-phenylene ether];
poly ( 2 -bromo - 6 -phenyl - 1 , 4 -phenylene ether ); poly ( 2 -methyl - 6-
phenyl - 1 , 4 - pheny l ene e ther ); p o l y ( 2 - phenyl - 1 , 4 - pheny l ene
ether~; poly(2-chloro-1,4-phenylene ether); poly(2-methyl-
1,4-phenylene ether); poly(2-chloro-6-ethyl-1,4-phenylene
ether); poly(2-chloro-6-bromo-1,4-phenylene ether);
poly(2,6-di-n-propyl-1,4-phenylene ether); poly(2-methyl-6-
isopropyl-1,4-phenylene ether); poly(2-chloro-6-methyl-1,4-
phenylene ether); poly(2-methyl-6-ethyl-1, 4-phenylene
ether); poly(2,6-dibromo-1,4-phenylene ether); poly(2,6-
dichloro-1, 4-phenylene ether); poly (2, 6-diethyl-1, 4-
phenylene ether); and poly(2,6-dimethyl-1,4-phenylene
ether). In addition to these homopolymers, also employable
are copolymers to be derived from two or more phenolic
compounds such as those to be used in producing the
homopolymers. Moreover, also employable are graft
copolymers and block copolymers composed o~ aromatic vinyl
compounds such as polystyrene, and polyphenylene ethers such
as those mentioned above. 0~ those, especially preferred is
poly(2,6-dimethyl-1,4-phenylene ether).
In view oi its effect o~ improving the impact
resistance of the article to be formed from the composition
o~ the invention, it is desirable that the polyphenylene
14
218~78
ether of the component (C) has an intrinsic viscosity of 0.~
dl/g or more, preferably 0.5 dl/g or more, as measured in
chloroform at 25 C. The content of the component (C~ in the
composition of the invention shall be from O . 5 to 10 parts
by weight, relative to 100 parts by weight of the component
(a) of (A) . If the content is less than O . 5 parts by
weight, the impact strength of the article to be formed from
the composition could not be improved satisfactorily.
However, if it is more than 10 parts by weight, the
shapability or moldability of the compositio~ will be
worsened. Preferably, the content of the component (C) is
from 1. O to 5 . O parts by weight relative to 100 parts by
weight of the c _ nn~nt (a) of (A) .
In order to further improve the toughness of the
article to be formed from the resin composition of the
invention, the composition may contain, if desired, a fourth
c .~nl~nt (D) of a styrene-olefin copolymer having a styrene
content of from 5 to 35 96 by weight. The component (D) must
be a styrene-olefin copolymer having high miscibility with
or a strong affinity for the component (b) of (A) .
Therefore, the styrene content of the copolymer must be from
5 to 35 % by weight. If its styrene content does not fall
within the defined range, the copolymer would not be
effective in improving the toughness of the article to be
formed from the composition of the invention.
~ 218~77~
The styrene-olefin copolymer for the component (D)
differs from that for the component (B) only in the styrene
content. Therefore, for the copolymers for the component
(D), those for the component (B) shall be referred to except
for the styrene content. Of these, preferred for the
component (D) are styrene-olefin diblock copolymers and
styrene-olefin triblock copolymers. Concretely, preferred
examples of the copolymers for the component (D) i~clude
styrene-butadiene block copolymer (SBR), hydrogenated
styrene-butadiene block copolymer (SEB, SEBC), styrene-
butadiene-styrene block copolymer (SBS), hydrogenated
styrene-butadiene-styrene block copolymer (SEBS), styrene-
isoprene block copolymer (SIR), hydrogenated styrene-
isoprene block copolymer (SEP), styrene-isoprene-styrene
block copolymer (SIS), hydrogenated styrene-isoprene-styrene
block copolymer (SEPS), and their modificates.
The component (D) may comprise one or more such
copolymers, either singly or as cn~h; nf~
The composition of the present invention may comprise
from 0 to 200 parts by weight, relative to 100 parts by
weight of the nnnlpnnf~nt (b) of (A), of the component (D).
Even if the content of the component (D) is more than 200
parts by weight, the toughness of the article to be formed
from the composition could not be improved so much.
Therefore, the addition of such a large amount of the
16
` 218~778
!-
component (D) to the composition is unfavorable in view of
the cost of the composition. Preferably, the content of the
component (D) in the composition is from 1 to 150 parts by
weight, more preferably from 5 to 150 parts by weight.
In order to improve the fluidity of the resin
composition of the invention and the toughness of the
article to be formed from the composition, still another
component (E) of a paraffinic oil, a paraffinic wax, a
mineral oil or a siloxanic oil may be added to the
composition, if desired. The component (E) must be highly
miscible with or have a strong affinity for the component
(b) of (A). If not, the toughness of the article to be
formed from the composition of the invention could not be
improved.
The component (E) of a paraffinic oil, a paraffinic
wax, a mineral oil or a ~;lr~ n;c oil ;nr1~ q, for example,
polyethylenic oligomers, polyethylenic waxes, polyolefinic
oligomers, polyolefinic waxes, heavy cycloparaffins, mineral
oils, fatty acid esters, esters of aliphatic, dibasic acids,
phthalates, aromatic carboxylates, phosphates,
polydimethylsiloxanes, dimethylsiloxane-diphenylsiloxane
copolymers, and polymethylphenylsiloxanes. o~ these,
preferred are polyethylenic oligomers, polyethylenic waxes,
mineral oils, polydimethylsiloxanes, dimethylsiloxane-
diphenylsiloxane copolymers, and polymethylphenylsiloxanes.
17
218~778
The component (E) may comprise one or more such
compounds, either singly or as c~mh; n -d
The composition of the present invention may comprise
from 0 to 200 parts by weight, relative to 100 parts by
weight of the component (b) of (A), of the component (E).
Even if the content of the component (E) is more than 200
parts by weight, any further effect o the component (E) of
improving the toughness of the article to be formed from the
composition could not be e~pected, but rather the modulus of
elasticity o~ the article would be unfavorably lowered.
Preferably, the content of the component (E) is from 1 to
150 parts by weight, more preferably from 5 to 100 parts by
weight .
If desired, the composition of the present invention
may comprise both the component (D) and the component (E).
The combination of the component (D) and the component (E)
is preferred to the single use of either the component (D)
or the component (E), since the former produces higher
improvement in the toughness of the article to be formed
from the composition of the invention. If desired, the
component (D) and/or the component (E) may be previously
mixed with the c~mr~nf~n~ (b) of (A) .
In order to much more increase the modulus of
elasticity and the heat resistance of the article to be
formed from the resin composition of the invention, it is
18
~ 218~778
advantageous to incorporate still another component (F) of
an inorganic filler into the composition. Various forms of
inorganic fillers can be employed herein, including, for
example, fibrous, granular and powdery ones. Fibrous
fillers include, for example, glass fibers, carbon fibers
and whiskers. The form or shape of the fibrous filler
includes, for example, clothes, mats, bound and cut fibers,
short fibers, filaments and whiskers. The bound and cut
fibers preferably have a length of from 0 . 05 to 50 mm and a
diameter of from 5 to 20 ,um.
Examples of granular or powdery fillers include talc,
carbon black, graphite, titanium dioxide, silica, mica,
calcium carbonate, calcium sulfate, barium carbonate,
magnesium carbonate, magnesium sulfate, barium sulfate,
hydroxysulfates, tin hydroxide, alumina, kaolin, silicon
carbide, metal powders, glass powder, glass flakes, and
glass beads. Of these, preferred are glass fillers, such as
glass powder, glass flakes, glass beads, glass filaments,
glass f ibers, glass rovings, and glass mats .
It is desirable that the inorganic filler is surface-
treated. For the surface treatment, used is a coupling
agent, by which the adhesiveness of the filler to resins is
improved. The coupling agent can be selected from any known
silane coupling agents, titanium coupling agents and others.
Above all, especially preferably used are aminosilanes and
19
218~78
.
epoxysilanes such as ~y-aminopropyltrimethoxysilane, N-,~-
(aminoethyl) -r-aminopropyltrimethoxysilane, ~y-
glycidoxypropyltrimethoxysilane, and ~- ( 3, 4 -
epoxycyclohexyll ethyltrimethoxysilane; and also isopropyltri (N-amidoethyl, aminoethyl) titanate.
The means of surface-treating the filler with any of
such coupling agents is not specifically defined, and any
known methods can be employed for the surface treatment.
For example, employable are a sizing method where a solution
or suspension of a coupling agent is applied to a filler as
a so-called sizing agent, and also a dry-mixing method, a
spraying method, an integral-blending method and a dry-
concentrating method where a Henschel mixer, a super mixer,
a V-shaped mixer or the like is used. Any of these methods
may be selected, depending on the shape of the f iller to be
surface-treated. Of these, preferably employed are a sizing
method, a dry-mixing method and a spraying method.
The coupling agent can be combined with a film-forming
substance for glass. ~he film-forming substance to be
combined is not specifically defined but includes, for
example, polyester-type, polyether-type, urethane-type,
epoxy-type, acryl-type and vinyl acetate-type polymers.
One or more inorganic fillers can be used for the
component (F), either singly or as ~ mh; nF~1 . The content of
the component (F) to be in the composition of the present
218~778
invention shall be from 0.5 to 350 parts by weight relative
to 100 parts by weight of (~ the resin component comprising
the component (A) and the component (s), (~) the resin
component comprising the component (A), the component (s)
and the component (C), ~) the resin component comprising :-
the component (A), the component (s), the component (C) and
the component (D), (~3 the resin component comprising the
component (A), the component (B), the component (C) and the
component (E), (~) the resin component comprising the
component (A), the component (B), the component (C), the
component (D) and the ~ rr~nf~nt ~E), (~) the resin component
comprising the component (A), the component (B) and the
component (D), (~) the resin component comprising the
component (A), the component (B) and the component (E), or
~) the resin component comprising the component (A), the
component (s), the component (D) and the component (E) . If
the content is less than 0.5 parts by weight, the effect of
the filler could not be attained. However, if it is more
than 350 parts by weight, the dispersibility of the filler :_
in the composition is worsened so that the composition is
disadvantageously difficult to shape or mold. Preferably,
the content of the inorganic filler is from 5 to 200 parts
by weight, more preferably from 10 to 150 parts by weight.
In order to improve the adhesiveness of the inorganic
filler to the resin components constituting the composition
21
~ 2184778
of the present invention, it is desirable to add, along with
the inorganic filler for the component (F), still another
component (G) of a polymer which is miscible with or has an
affinity for the styrene-based polymer having a syndiotactic
configuration for the component (a) of (A) and which has a
polar group, to the composition.
The polymer which is miscible with or has an affinity
for the component (a) of (A), as referred to herein, is a
polymer having therein a polymeric chain that is miscible
with or has an affinity for the component (a) of (A). The
polymer of this type includes, for example, polymers having,
in the main chain, the block chain or the graf t chain, any
of syndiotactic polystyrene, atactic polystyrene, isotactic
polystyrene, styrenic copolymer, polyphenylene ether,
polyvinyl methyl ether and the like. The polar group which
the polymer shall have is not specifically defined, and may
be any and every group capable of improving the adhesiveness
of the inorganic filler for the component (F) to the resin
components constituting the composition of the invention.
Examples of the polar group include residues of acid
anhydrides, carboxylic acids, carboxylates, carboxylic acid
chlorides, carboxylic acid amides, salts of carboxylic
acids, sulfonic acids, sulfonates, sulfonic acid chlorides,
sulfonic acid amides, or salts of sulfonic acids; and also
22
` ~ 218~778
epoxy groups, amino groups, imido groups and oxazoline
groups .
Specific examples of the component (G) include styrene-
maleic anhydride copolymer (S~qA~, styrene-glycidyl
methacrylate copolymer, terminal carboxylic acid-modif ied
polystyrene, t~rm;n~7 epoxy-modified polystyrene, terminal
oxazoline-modified polystyrene, terminal amino-modified
polystyrene, sulfonated polystyrene, styrene-based ionomer,
styrene-methyl methacrylate graft polymer, (styrene-glycidyl
methacrylate) -methyl methacrylate graf t polymer, acid-
modified acryl-styrene graft polymer, (styrene-glycidyl
methacrylate)-styrene graft polymer, polybutylene
terephthalate-polystyrene graft polymer; as well as
modified, styrene-based polymers such as maleic anhydride-
modified syndiotactic polystyrene, fumaric acid-modified
syndiotactic polystyrene, glycidyl methacrylate-modified
syndiotactic polystyrene, and amine-modified syndiotactic
polystyrene; and also modified polyphenylene ether-based
polymers such as (styrene-maleic anhydride)-polyphenylene
ether graft polymer, maleic anhydride-modified polyphenylene
ether, fumaric acid-modified polyphenylene ether, glycidyl
methacrylate-modified polyphenylene ether, and amine-
modified polyphenylene ether. Of these, especially
preferred are modified syndiotactic polystyrenes and
23
218~778
.
modif ied polyphenylene ethers . These can be used either
singly or as ~n~nh; nP~l,
~ he polar group content of the polymer is preferably
from 0.01 to 20 96 by weight, more preferably from 0.05 to 10
96 by weight. If the content is less than 0 . 01 96 by weight,
a large amount of the polymer for the component (G) must be
added to the composition in order to attain the intended
adhesiveness of the inorganic filler to the resin components
constitutirg the composition. Such is unfavorable, since
the mechanical properties, the heat resistance and the
shapability of the composition are often lowered. If, on
the other hand, the content is more than 20 % by weight, the
miscibility of the polymer with the component (a) of (A)
would be lowered and such is also unfavorable.
Modified sy~diotactic polystyrenes are preferably used
for the component (G), which are referred to below. SPS to
be modified is not specifically defined. Any of the
polymers as referred to for the component (a) of (A) can be
used to obtain modified polymers. In view of the
miscibility of the modified polymers with the component (a)
of (A), preferably used are styrene homopolymers or styrene-
substituted styrene copolymers. For the latter copolymers,
the compositional proportions of the constitutive monomers
are not specifically defined. E~owever, the content of the
substituted styrene units in the copolymers is preferably 50
24
218~778
mol96 or less. If it is more than 50 mol%, the miscibility
of the modified copolymers with the component (a) of (A)
would be lowered and such is unfavorable. The substituted
styrene includes, for example, alkylstyrenes such as
methylstyrene, ethylstyrene, isopropylstyrene, tert-
butylstyrene, and vinylstyrene; halogenostyrenes such as
chlorostyrene, bromostyrene, and fluorostyrene;
halogenoalkylstyrenes such as chloromethylstyrene; and
alkoxystyrenes such as methoxystyrene, and ethoxystyrene.
These substituted styrenes can be used either singly or as
c~,mh; nf~.1
As the modifying agent to be used for modifying SPS
such as that mentioned hereinabove, employable is a compound
having both an ethylenic double bond and a polar group in
one molecule. The compound includes, for example, maleic
acids such as maleic anhydride, maleic acid, maleates,
maleimide and its N-substituted derivatives, and salts of
maleic acid; fumaric acids such as fumaric acid, fumarates,
and salts of fumaric acid; itaconic acids such as itaconic
anhydride, itaconic acid, itaconates, and salts of itaconic
acid; acrylic acids such as acrylic acid, acrylates, acrylic
acid amides, and salts o~ acrylic acid; and methacrylic
acids such as methacrylic acid, methacrylates, methacrylic
acid amides, salts of methacrylic acid, and glycidyl
methacrylate. Of these, especially preferred are maleic
4778
anhydride, fumaric acid, fumarates and glycidyl
methacrylate. The modifying agent can comprise one or more
such compounds either singly or as ~ ' ;nf.~
To obtain modified SPS, for example, SPS such as that
mentioned above is reacted with a modifying agent such as
that mentioned above, in the presence or absence o~ a
solvent or any other resin. The modification is not
specifically defined but can be conducted in accordance with
any known methods. For example, employable are a method of
melting, kneading and reacting the components at a
temperature falling between 150-C and 350 C, using, for
example, a roll mill, a sambury mixer or an extruder, and a
method of reacting the components under heat in a solvent
such as benzene, toluene or xylene. In order to promote the
reaction, it is effective to add to the reaction system, a
radical-generating agent such as benzoyl peroxide, di-t-
butyl peroxide, dicumyl peroxide, t-butyl peroxybenzoate,
azobisisobutyronitrile, azobisisovaleronitrile, or 2, 3-
diphenyl-2, 3-dimethylbutane. One preferred method for the
modif ication is to melt and knead the component in the
presence of such a radical-generating agent. During the
modification, if desired, any other resin can be added to
the reaction system. 26
. 2184778
.
Of the modified SPS thus obtained, especially preferred
are maleic anhydride-modified SPS, fumaric acid-modified SPS
and fumarate-modified SPS.
Modified polyphenylene ethers are also preierably used
for the component (G), which can be obtained by modifying
known polyphenylene ethers with a modifying agent. The
polyphenylene ethers to be modified are not specifically
defined, and any of the polymers as referred to hereinabove
for the component (C) can be used. Above all, preferred is
poly (2, 6-dimethyl-1, 4-phenylene ether) .
The modifying agents usable for the modification of
polyphenylene ethers may be the same as those referred to
hereinabove for the modification of SPS. In particular,
preferably used are maleic anhydride, fumaric acid,
fumarates and glycidyl methacrylate. One or more such
modifying agents can be used either singly or as combined.
The modification of polyphenylene ethers can be conducted in
the same manner as that mentioned hereinabove for the
modification of SPS.
Of the modified polyphenylene ethers thus obtained,
especially preierred are maleic anhydride-modified
polyphenylene ether, fumaric acid-modiied polyphenylene
ether, and fumarate-modified polyphenylene ether.
The composition of the present invention may comprise
one or more polymers having a polar group or the component
27
~ 218~778
(G), either singly or as combined. The content o~ the
component (G) to be in the composition shall be from O.1 to
10 parts by weight relative to 100 parts by weight of (~)
the resin component comprising the component (A) and the
component (B), @) the resin component comprising the
component (A), the component (B) and the component (C), (~
the resin component comprising the component (A), the
component (B), the component (C) and the component (D), (~)
the resin component comprising the component (A), the
component (B), the component (C) and the compo~ent (E), ~
the resin component comprising the component (A), the
component (B), the component (C), the component (D) and the
component (E), OE) the resin component comprising the
component (A), the component (B) and the component (D), @)
the resin component comprising the component (A), the
component (B) and the component (E), or (~) the resin
component comprising the component (A), the component (B),
the component (D) and the component (E) If the content is
less than O 1 parts by weight, the adhesiveness of the
inorganic filler to the resin components could not be
satisfactorily improved. However, if it is more than 10
parts by weight, the heat resistance and the ~ Ar~h;1;ty Of
the composition would be lowered In view of the
adhesiveness of the inorganic f iller to the resin components
and of the heat resistance and the shapability of the
28
2184778
.
composition, the content of the component (G) in the
composition is preferably from 0.5 to 8 parts by weight,
more preferably from 1 to 5 parts by weight
The resin composition of the present invention may
optionally contain, if desired, any known additives, such as
a nucleating agent, an antioxidant, a plasticizer, a flame
retardant, a f lame retardant aid, a release agent, a
pigment, carbon black, an antistatic agent, and other rubber
components and thermoplastic resins, provided that such
additives do not detract from the objects of the present
invention .
The nucleating agent includes, for example, metal salts
of carboxylic acids, such as aluminium di (p-tert-
butylbenzoate); metal salts of phosphoric acid such as
sodium methylenebis(2,4-di-t-butylphenol) acid phosphate;
and also talc and phthalocyanine derivatives. The
antioxidant can be selected from any known phosphorus-
containing, phenolic, or sulfur-containing antioxidants.
The plasticizer can be selected from any known ones,
including, for example, polyethylene glycol, polyamide
oligomers, ethylenebis-stearoamide, and polyethylene
oligomers .
The flame retardant can be selected from any known
ones, including, for example, brominated polymers such as
brominated polystyrenes, brominated syndiotactic
29
218~778
polystyrenes, and brominated polyphenylene ethers; and
brominated aromatic compounds such as brominated
diphenyl~lk~n-~c, and brominated diphenyl ethers. The flame
retardant aid can be selected from any known ones,
including, for example, antimony compounds such as antimony
trioxide. The release agent can be selected from any known
ones, including, for example, polyethylene waxes, silicone
oils, long-chain carboxylic acids, and metal salts of long-
chain carboxylic acids. One or more such additives can be
used either singly or as c ~ ;n~
Specific examples of rubber-like elastic materials
which can be added to 'che composition of the present
invention include natural rubber, polybutadiene,
polyisoprene, polyisobutylene, neoprene, polysulfide rubber,
Thiokol rubber, acrylic rubber, urethane rubber, silicone
rubber, epichlorohydrin rubber, and also core/shell type,
granular, elastic rubber substances, such as butadiene-
acrylonitrile-styrene core/shell rubber (ABS), methyl
methacrylate-butadiene-styrene core/shell rubber (MBS),
methyl methacrylate-butyl acrylate-styrene core/shell rubber
(MAS), octyl acrylate-butadiene-styrene core/shell rubber
(MABS ), alkyl acrylate-butadiene-acrylonitrile-styrene
core/shell rubber (AABS), butadiene-styrene core/shell
rubber (SBR), methyl methacrylate-butyl acrylate-siloxane
and other siloxane-containing core/shell rubbers, as well as
~ 21~778
modificates to be obtained by modifying these rubbers. One
or more such rubber-like elastic materials can be used
either sin~ly or as ~-~ ' ;n~d.
Any known thermoplastic resins, for example, as
selected from polystyrene resins such as polystyrene, ~IIPS,
ABS, and AS; polyester resins such as polycarbonates,
polyarylates, polyethylene terephthalate, and polybutylene
terephthalate; polyamide resins such as polyamide 6,
polyamide 66, polyamide 46, polyamide 12, and aromatic
polyamides; and PPS, can be added to the composition of the
present invention. One or more such thermoplastic resins
can be used either singly or as cr~mh; n~.tl .
The method for preparing the resin composition o~ the
present invention is not specif ically def ined . The
composition can be prepared by any known methods. For
example, the components (a) and (b) of (A), the component
(B) and optionally the component (C), the C~m}~n~nt (D), the
component (E), the component (F), the component (G) and
other various additives are melted and kneaded, using a
ribbon blender, a Henschel mixer, a sambury mixer, a drum
tumbler, a single-screw extruder, a twin-screw extruder, a
co-kneader, a multi-screw extruder or the like mixing
device, to obtain a resin composition o~ the present
invention .
31
. 2184778
.
The resin composition of the present invention can be
shaped into articles having excellent physical properties,
and the method i~or shaping it is not defined. For example,
the composition can be shaped into various articles through
injection molding, into sheets or films through extrusion
molding, into containers or trays through extrusion molding
combined with thermal molding, into monoaxially or h;~ lly
stretched films or sheets through extrusion molding combined
with stretching, or into fibrous articles through Sp;nn;n~,
The present invention is described in more detail
hereinunder with reference to the following examples, which,
however, are not intended to restrict the scope of the
invention. The physical properties of the samples as
obtained in the ~ollowing examples were det~rm; nf~ according
to the methods mentioned below.
(1) Izod impact strength (with notch):
This was obtained in accordance with JIS ~-7110.
(2) Tensile elongation:
This was obtained in accordance with JIS K-7113.
(3) Surface layer peeling resistance:
Each sample was visually observed and ranked in three,
as ~ollows:
A: Very good
B: Good
C: Not good
32
218~778
Production Example 1: Production of SPS
1. 0 liter of pure styrene and 1 mmol of triethyl
aluminium were put into a 2-liter reactor and heated at
80 C. Next, 16.5 ml of a pre-mixed catalyst (comprising 90
mols of pentamethylcyclopentadienyl titanium trimethoxide,
90 ,umols of dimethylanilinium
tetrakis (pentafluorophenyl)borate, 29 .1 mmols of toluene and
1. 8 mmols of triisobutyl aluminium) was added thereto, and
the monomer was polymerized at 80 C for 5 hours . Af ter the
polymerization, the product was washed plural times with
methanol and dried. Thus was obtained 380 y of a polymer.
The weight average molecular weight of the polymer was
measured through gel permeation chromatography at 13 0 C
using a solvent of 1,2,4-trichlorobenzene, to be 300,000.
The ratio of weight average molecular weight/number average
molecular weight of the polymer was 2.70. It was confirmed
that the polymer obtained herein is SPS from the results of
the measurement of its melting point and the 13C-NMR
analysis thereof.
Production Example 2: Production of Maleic Anhydride-
Modified SPS
One kg of SPS as produced in Production Example 1, 30 g
of maleic anhydride and 10 g of a radical-generating agent
of cumene hydroxyperoxide were dry-blended, then melted and
kneaded through a 3 0-mm twin-screw extruder at a screw
33
218~778
.
revolution of 200 rpm and at a temperature of 300 C. The
strands thus extruded out were cooled and then pelletized to
obtain pellets of a maleic anhydride-modified SPS
To measure the degree of modification o~ the product,
one g of the modified SPS was dissolved in ethylbenzene,
then re-precipitated in methanol and collected The thus-
collected polymer was subjected to Soxhlet extraction using
methanol and then dried. The degree of modification of the
polymer was obtained from the intensity o~ the carbonyl
absorption in its IR spectrum and from its titration, to be
1.04 % by weight.
Production Example 3: Production of Fumaric Acid-Modified
Polyphenylene Ether
One kg of polyphenylene ether (having an intrinsic
viscosity of 0.45 dl/g in chloroform at 25 C), 30 g of
fumaric acid and 20 g of a radical-generating agent of 2,3-
dimethyl-2, 3-diphenylbutane (produced by Nippon Oils & Fats
Co., ~td. under the trade name of nNofmer sC~ ) were dry-
blended, then melted and extruded through a 30-mm twin-screw
extruder at a screw revolution of 200 rpm and at a
temperature of 300'C. The temperature of the resin being
extruded was about 330 c. The strands thus extruded out
were cooled and then pelletized to obtain pellets of a
fumaric acid-modified polyphenylene ether. To measure the
degree of modification of the product, one g of the modified
34
218~778
.
polyphenylene ether was dissolved in ethylbenzene, then re-
precipitated in methanol and collected. The thus-collected
polymer was subjected to Soxhlet extraction using methanol
and then dried. The degree of modification of the polymer
was obtained from the intensity of the carbonyl absorption
in its IR spectrum and from its titration, to be 1. 6 96 by
weight .
Example 1:
50 parts by weight of the syndiotactic polystyrene as
prepared in Production Example 1 (having a weight average
molecular weight of 300, 000 and a ratio of weight average
molecular weight/number average molecular weight of 2.70)
(this corresponds to the component (a) of (A) ), 50 parts by
weight of EPM (produced by Japan Synthetic ~ubber Co., Ltd.
under the trade name of "EP-07P" ) (this corresponds to the
component (b) of (A) ), and, relative to 100 parts by weight
of the sum of these two, 30 parts by weight of SEBS
(produced by Asahi Chemical Industry Co., Ltd. under the
trade name of "Tuftec H-1081" ) (this corresponds to the
component (B) ), 0.5 parts by weight of a nucleating agent of
sodium methylenebis(2,4-di-t-butylphenol) acid phosphate
(produced by Asahi Denka Co., Ltd. under the trade name of
"NA-ll"), 0.1 parts by weight of an antioxidant of (2,6-di-
t-butyl-4-methylphenyl)pentaerythritol diphosphite (produced
by Asahi Denka Co ., ~td. under the trade name of " PEP-3 6 " ),
2184778
.
and 0 .1 parts by weight of tetrakis (methylene-3- ~3 ~, 5 ' -di-t-
butyl-4 ~-hydroxyphenyl) ) propionate (produced by Adeka Argus
Co ., Ltd. under the trade name of "MARK AO 60 ' ) were dry-
blended in a Henschel mixer, then melted, kneaded and
pelletized through a twin-screw extruder. The pellets thus
obtained were molded through injection molding to obtain
test pieces for an Izod impact test and a tensile elongation
test. These test pieces were tested to measure their Izod
impact strength and tensile elongation. The results
obtained are shown in Table 1 below.
Examples 2 to 43, Comparative Examples 1 to 3 0:
The same process as in Example 1 was repeated except
that the components (a) of (A), (b) of (A), (B), (C), (D)
and (E) as shown in Table 1 below were used herein. The
results obtained are shown in Table l
As is known from Table 1, the samples comprising the
component (B) having a higher styrene content had much more
increased impact strength and elongation than those
comprising the component (B) having a lower styrene content.
It is also known therefrom that the samples containing the
component (C), the component (D) and the component (E) had
more increased impact strength and elongation than those not
containing them.
Example 44:
36
2184778
.
50 parts by weight of the syndiotactic polystyrene as
prepared in Production Example 1 (having a weight average
molecular weight of 300,000 and a ratio of weight average
molecular weight/number average molecular weight of 2.70)
(this corresponds to the component (a) of (A) ), 50 parts by
weight of EPM (produced by ~apan Synthetic Rubber Co., Ltd.
under the trade name of 'EP-07P'~ his corresponds to the
component (b) of (A) ), and, relative to 100 parts by weight
of the sum of these two, 30 parts by weight of SEBS
(produced by Asahi Chemical Industry Co., Ltd. under the
trade name of "Tuftec H-1081" ) (this corresponds to the
component (B) ), 0 . 5 parts by weight of a nucleating agent of
sodium methylenebis(2,4-di-t-butylphenol) acid phosphate
(produced by Asahi Denka Co., Ltd. under the trade name of
"NA-ll"), 0.1 parts by weight of an antioxidant of (2,6-di-
t-butyl-4-methylphenyl)pentaerythritol diphosphite (produced
by Asahi Denka Co, Ltd. under the trade name of "PEP-36n),
and 0 1 parts by weight of tetrakis (methylene-3- (3 ', 5 ~ -di-t-
butyl -4 ~ -hydroxyphenyl ) ) propionate (produced by Adeka Argus
Co , Ltd. under the trade name of "MARK AO 60 " ) were dry-
blended in a Xenschel mixer, then melted, kneaded and
pelletized through a twin-screw extruder while adding
thereto 55.7 parts by weight of glass fibers (produced by
Asahi Fiber Glass Co ., Ltd. under the trade name o~ "FT-712
- 10 1Im/3 mm) (this corresponds to t~e component (F) ) .
37
2184778
The pellets ~hus obtained were molded through injection
molding to obtain test pieces for an Izod impact test and a
tensile elongation test. These test pieces were tested to
measure their Izod impact strength and tensile elongation.
The results obtained are shown in Table 2 below.
Examples 45 to 96, Comparative Examples 3 to 70:
The same process as in Example 44 was repeated except
that the components (a) of (A), (b) of (A), (B), (C), (D),
(E), (F) and (G) as shown in Table 2 below were used herein.
The results obtained are shown in Table 2.
As is known from Table 2 where all the samples tested
contained the inorganic filler of the component (F), the
samples comprising the component (B) having a higher styrene
content had much more increased impact strength and
elongation than those comprising the component (B) having a
lower styrene content. It is also known therefrom that the
samples containing the component (C), the component (D), the
component (E) and the component (G) had more increased
impact strength and elongation than those not containing
them .
As has been described hereinabove, the impact-
resistant, polystyrenic resin composition of the present
invention has good shapability and can be formed into
articles having high heat resistance, high impact strength,
high tensile elongation, and a high modulus of elasticity.
38
~ 2184778
Without being limited by the means of shaping it, the
composition of t~e present invention can be shaped into
articles having such good physical properties. For example,
the impact-resistant, polystyrenic resin composition of the
present invention can be molded into various articles
through injection molding, into sheets and films through
extrusion molding, into containers or trays through
extrusion molding combined with thermal molding, into
m~noi~ 1 ly or biaxially stretched films or sheets through
extrusion molding combined with stretching, or into fibrous
articles through spinning.
39
. 2184778
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~ 2184778
Notes:
SPS: Obtained in Production Example 1.
EP07P: EPR produced by Japan Synthetic Rubber Co,
Ltd .
EPl81SP: EPD~I produced by Japan Synthetic Rubber Co,
Ltd .
E-185G: b-PP produced by Idemitsu Petrochemical Co.,
Ltd .
L0134N: LLDPE produced by Idemitsu Petroc~emical Co.,
Ltd .
Tuftec Hl081: SEBS produced by Asahi Chemical Industry
Co., Ltd.
Tuf tec H1041: SEBS produced by Asahi Chemical Industry
Co., Ltd.
Septon 2104: SEPS produced by l~uraray Co., Ltd
Septon 2002: SEPS produced by ECuraray Co., Ltd.
Septon 8006: SEBS produced by Kuraray Co., Ltd.
Dynaron HBS576: SEsC produced by Japan Synthetic
Rubber Co., Ltd
PPE: Poly~2,6-dimethyl-1,4-phenylene ether) having an
intrinsic viscosity of 0 . 55 dl/g in chloro~orm at 25 C.
PW 380: Paraffin oil produced by Idemitsu ~osan Co,
Ltd
SH 200: Silicone oil produced by Toray Dow Corning
Silicone Co., Ltd.
94
~ 218~778
FT 712: Glass fiber ~aving a length o~ 3 mm and a
diameter of 10 ,um, produced by Asahi Fiber Glass Co.,
~td.
As has been described in detail hereinabove, the
syndiotactic polystyrenic resin composition of the present
invention can be formed into articles having good heat
resistance, a high modulus of elasticity and greatly
improved toughness. In addition, the articles are
advantageous in that their surface layers are hardly peeled.
Therefore, the resin composition of the present
invention is favorably used in forming various materials for
industrial use, for example, electric and electronic
materials (e.g., connectors, substrates ~or printed
circuits ), industrial construction materials , car parts
( e . g ., connectors to be mounted on cars , wheel caps ,
cylinder head covers), household appliances, various machine
parts, pipes, sheets, trays, f i lms, etc .
While the invention has been described in detail and
with reference to specific embodiments thereof, it will be
apparent to one skilled in the art that various changes and
modifications can be made therein without departing from the
spirit and scope thereo~.
~5
