Polyolefin resin composition

The present invention discloses a polyolefin resin composition comprising a specific cycloolefin-based polymer (a), a graft-modified elastomer (b) and a compound (c) having one amino group in the molecule, and containing, based on the total amount of the components (a), (b) and (c), 50 to 95% by weight of the component (a), 1 to 50% by weight of the component (b) and 0.01 to 45% by weight of the component (c). This polyolefin resin composition is improved particularly in mechanical properties such as impact strength, etc., while retaining excellent properties of the cycloolefin-based polymer (a).

TECHNICAL FIELD 
The present invention relates to a polyolefin resin composition. More 
specifically, it relates to a polyolefin resin composition comprising a 
cycloolefin-based polymer (a), a graft-modified elastomer (b) and an amino 
compound (c) and being excellent in impact resistance. 
TECHNICAL BACKGROUND 
Conventional polyolefins are resins excellent in chemical resistance and 
solvent resistance, but cannot be said to have sufficient rigidity and 
heat resistance, when their crystallinity is low. 
In order to improve polyolefins in heat resistance and rigidity, there is 
therefore employed a method in which a nucleating agent is added or a 
polyolefin in a molten state is gradually cooled to increase the 
crystallinity. However, the effect thereof cannot be said to be 
satisfactory. 
Apart from such conventional polyolefins, it is reported that a copolymer 
obtained by reaction of ethylene with a bulky monomer is excellent over 
conventional polyolefins in various properties such as heat resistance, 
etc. (U.S. Pat. No. 2,883,372 and Japanese Patent Publication No. 
14910/1971). 
The assignee of the present application already found that a cycloolefin 
random copolymer obtained by copolymerization of a specific cycloolefin as 
a bulky monomer and ethylene is excellent in heat resistance, thermal 
aging resistance, solvent resistance, dielectric properties and rigidity. 
On the basis of this finding, the assignee of the present application has 
already proposed inventions of random copolymers obtained from specific 
cycloolefins (Japanese Laid-Open Patent Publications Nos. 168708/1985, 
98780/1986, 115912/1986, 115916/1986, 120816/1986 and 252407/1987). 
DISCLOSURE OF THE INVENTION 
It is an object of the present invention to further improve such a resin 
composition containing a cycloolefin-based resin as mentioned above in 
mechanical properties such as impact strength. 
It is another object of the present invention to provide a cycloolefin 
random copolymer-containing resin composition being further improved 
particularly in mechanical properties such as impact strength without 
impairing excellent properties of cycloolefin-based resins. 
Other objects and advantages of the present invention will be apparent from 
the following description. According to the present invention, the above 
objects and advantages of the present invention are achieved by a 
polyolefin resin composition comprising: 
(a) at least one cycloolefin-based polymer selected from the group 
consisting of a homopolymer (a1) derived from one of cycloolefins of the 
following formula (I), 
##STR1## 
(wherein n is 0 or 1, m is 0 or a positive integer, q is 0 or 1, each of 
R.sup.1 to R.sup.18, R.sup.a and R.sup.b is, independently of the other, 
an atom or a group selected from the class consisting of a hydrogen atom, 
a halogen atom and a hydrocarbon group, 
the two of R.sup.15 to R.sup.18 may bond to each other to form a monocyclic 
or polycyclic group which may have a double bond, and further, a 
combination of R.sup.15 and R.sup.16 or a combination of R.sup.17 and 
R.sup.18 may form an alkylidene group), 
a copolymer (a2) derived from said cycloolefins, a hydrogenation polymer 
(a3) of the homopolymer (a1) or the copolymer (a2), and a 
cycloolefin/ethylene random copolymer (a4) composed of a polymer unit 
derived from said cycloolefins and a polymer unit of ethylene, 
(b) an elastomer being graft-modified with an unsaturated carboxylic acid 
or a derivative thereof and having a tensile modulus, at 23.degree. C., of 
0.1 to 2,000 kg/cm.sup.2, and 
(c) a compound having one amino group in the molecule, 
(d) the polyolefin resin composition containing, per 100 parts by weight of 
the total amount of the component (a), the component (b) and the component 
(c), 50 to 95 parts by weight of the component (a), 1 to 50 parts by 
weight of the component (b) and 0.01 to 45 parts by weight of the 
component (c). 
The polyolefin resin composition of the present invention basically 
comprises a cycloolefin-based polymer (a), a graft-modified elastomer (b) 
and a compound (c) having one amino group in the molecule as described 
above. The composition of the present invention can provide molded 
articles being improved particularly in mechanical properties such as 
impact strength and in surface gloss without impairing excellent 
properties of cycloolefin-based resins. 
The polyolefin resin composition of the present invention will be 
specifically described hereinafter. 
The polyolefin resin composition according to the present invention is a 
composition composed basically of a cycloolefin-based polymer (a), a 
graft-modified elastomer (b) and a specific, amino group-containing 
compound (c). 
The component (a) used in the present invention, i.e., the 
cycloolefin-based polymer, is selected from the class consisting of a 
homopolymer (a1) derived from one of cycloolefins of the above formula 
(I), a copolymer (a2) derived from said cycloolefins, a hydrogenation 
polymer of the homopolymer (a1) or the copolymer (a2) and a 
cycloolefin/ethylene random copolymer (a4) composed of a polymer unit 
derived from said cycloolefins and a polymer unit of ethylene. These 
cycloolefin-based polymers may be used alone or in combination of two or 
more. 
In the above formula (I), n is 0 or 1, m is 0 or a positive integer, and q 
is 0 or 1. 
Each of R.sup.1 to R.sup.18, R.sup.a and R.sup.b is, independently of the 
other, is an atom or a group selected from the class consisting of a 
hydrogen atom, a halogen atom and a hydrocarbon group. The halogen atom 
includes, for example, a fluorine atom, a chlorine atom, a bromine atom 
and an iodine atom. The hydrocarbon group preferably includes, for 
example, an alkyl group having 1 to 20 carbon atoms and a cycloalkyl group 
having 3 to 15 carbon atoms. Examples of the alkyl group are preferably 
methyl, ethyl, propyl, isopropyl, amyl, hexyl, octyl, decyl, dodecyl and 
octadecyl. The cycloalkyl group preferably is, for example, cyclohexyl. 
In the above formula (I), R.sup.15 and R.sup.16, R.sup.17 and R.sup.18, 
R.sup.15 and R.sup.17, R.sup.16 and R.sup.18, R.sup.15 and R.sup.18, or 
R.sup.16 and R.sup.17 may bond to each other (jointly with each other) to 
form a monocyclic or polycyclic group. And, these monocyclic and 
polycyclic groups may have a double bond. 
Further, R.sup.15 and R.sup.16, or R.sup.17 and R.sup.18 may form an 
alkylidene group. Such an alkylidene group preferably includes an 
alkylidene group having 2 to 20 carbon atoms. Examples of such an 
alkylidene group are preferably an ethylidene group, a propylidene group 
and an isopropylidene group. 
The intrinsic viscosity [.eta.] of the above cycloolefin-based resins, 
measured in decalin at 135.degree. C., is preferably in the range of 0.3 
to 2.0 dl/g, more preferably in the range of 0.4 to 1.2 dl/g. The 
softening temperature (TMA) thereof, measured with a thermal mechanical 
analyzer, is preferably in the range of 70.degree. to 200.degree. C., more 
preferably in the range of 100.degree. to 180.degree. C. Further, the 
glass transition temperature (Tg) thereof is preferably in the range of 
50.degree. to 190.degree. C., preferably in the range of 80.degree. to 
170.degree. C., and the crystallinity thereof, measured by an X-ray 
diffraction method, is preferably in the range of 0 to 20%, more 
preferably in the range of 0 to 2%. 
Among the above cycloolefin-based resins, the polymer (a1), the copolymer 
(a2) and the hydrogenation polymers (a3) of these are basically formed of 
ring-opening polymerization polymers derived from cycloolefins. 
The polymer (a1) and the copolymer (a2) can be produced, for example, by 
(co)polymerizing cycloolefins of the above formula (I) in the presence of 
a catalyst comprising any one of a halide of a metal such as ruthenium, 
rhodium, palladium, osmium, indium or platinum; nitrate; and an 
acetylacetone compound and a reducing agent; or 
a catalyst comprising either a halide of a metal such as titanium, 
palladium, zirconium or molybdenum or an acetylacetone compound and an 
organoaluminum. 
The hydrogenation polymer (a3) can be produced, for example, by reducing 
the above-obtained ring-opening polymerization polymer of a cycloolefin, 
(a1) or (a2), with hydrogen in the presence of a hydrogenating catalyst. 
The cycloolefin/ethylene random copolymer (a4) can be produced, for 
example, by copolymerizing ethylene and an unsaturated monomer of the 
above formula (I) in a liquid phase in the presence of a catalyst. 
The cycloolefins of the above formula (I) can be easily produced by 
condensing cyclopentadienes and corresponding olefins or corresponding 
cycloolefins under a Diels-Alder reaction. 
That is, the cycloolefins of the above formula (I), used in the present 
invention, specifically include the following compounds: 
Bicyclo[2.2.1]hept-2-enes, 
Tetraccyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecenes, 
Hexacyclo[6.6.1.1.sup.3,6.1.sup.10,13.0.sup.2,7.0.sup.9,14 
]-4-heptadecenes, 
Octacyclo[8.8.0.1.sup.2,9.1.sup.4,7.1.sup.11,18.1.sup.13,16.0.sup.3,8.0.sup 
.12,17 ]-5-docosenes, 
Pentacyclo[6.6.1.1.sup.3,6.0.sup.2,7.0.sup.9,14 ]-4-hexadecenes, 
Heptacyclo-5-eicosenes, 
Heptacyclo-5-heneicosenes, 
Tricyclo[4.3.0.1.sup.2,5 ]-3-decenes, 
Tricyclo[4.4.0.1.sup.2,5 ]-3-undecenes, 
Pentacyclo[6.5.1.1.sup.3,6.0.sup.2,7.0.sup.9,13 ]-4-pentadecenes, 
Pentacyclopentadecadienes, 
Pentacyclo[4.7.0.1.sup.2,5.0.sup.8.13.1.sup.9,12 ]-3-pentadecenes, 
Heptacyclo[7.8.0.1.sup.3,6.0.sup.2,7.1.sup.10,17.0.sup.11,16.1.sup.12,15 
]-4-eicosenes, 
Nonacyclo[9.10.1.1.sup.4,7.0.sup.3,8. . . 
.0.sup.2,10.0.sup.12,21.1.sup.13,20.0.sup.14,19.1.sup.15,18 
]-5-pentacosenes, 
Petacyclo[4.8.4.sup.2,5.0.sup.8,13.1.sup.9,12 ]-3-hexadecenes, 
Heptacyclo[8.8.0.0.sup.3,8.1.sup.4,7.1.sup.11,18.0.sup.12,17.1.sup.13,16 
]-5-heneicosenes, and 
Nonacyclo[10.10.1.0.sup.2,11.0.sup.4,9.1.sup.5,8.0.sup.13,22.1.sup.14,21.0. 
sup.15,20.1.sup.16,19 ]-6-hexacosenes. 
Specific examples of the above compounds are as follows: 
Bicyclo[2.2.1]hept-2-enes; 
bicyclo[2.2.1]hept-2-ene 
##STR2## 
6-methylbicyclo[2.2.1]hept-2-ene, 5,6-dimethylbicyclo[2.2.1]hept-2-ene, 
1-methylbicyclo[2.2.1]hept-2-ene, 
6-ethylbicyclo[2.2.1]hept-2-ene, 
6-n-butylbicylo[2.2.1]hept-2-ene, 
6-isobutylbicyclo[2.2.1]hept-2-ene, and 
7-methylbicyclo[2.2.1]hept-2-ene: 
Tetraccyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecenes; 
tetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene 
##STR3## 
5,10-dimethyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
2,10-dimethyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
11,12-dimethyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
2,7,9-triemthyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
9-ethyl-2,7-dimethyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
9-isobutyl-2,7-dimethyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
9,11,12-trimethyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
9-ethyl-11,12-dimethyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
9-isobutyl-11,12-dimethyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 
]-3-dodecene, 
5,8,9,10-tetramethyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-methyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-ethyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-propyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-hexyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-stearyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8,9-dimethyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-ethyl-9-methyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-chlorotetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-bromotetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-fluorotetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8,9dichlorotetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-cyclohexyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-isobutyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-butyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-ethylidenetetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-ethylidene-9-methyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-ethylidene-9-ethyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-ethylidene-9-isopropyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-ethylidene-9-butyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-n-propylidenetetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-n-propylidene-9-methyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-n-propylidene-9-ethyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-n-propylidene-9-isopropyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 
]-3-dodecene, 
8-n-propylidene-9-butyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-isopropylidenetetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-isopropylidene-9-methyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 
]-3-dodecene, 
8-isopropylidene-9-ethyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene, 
8-isopropylidene-9-isopropyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 
]-3-dodecene, 
8-isopropylidene-9-butyltetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]-3-dodecene: 
Hexacyclo[6.6.1.1.sup.3,6.1.sup.10,13.0.sup.2,7.0.sup.9,14 ]-4-heptadecene; 
hexacyclo[6.6.1.1.sup.3,6.1.sup.10,13.0.sup.2,7.0.sup.9,14 ]-4-heptadecene 
##STR4## 
12-methylhexacyclo-[6.6.1.1.sup.3,6.1.sup.10,13.0.sup.2,7.0.sup.9,14 
]-4-heptadecene, 
12-ethylhexacyclo-[6.6.1.1.sup.3,6.1.sup.10,13.0.sup.2,7.0.sup.9,14 
]-4-heptadecene, 
12-isobutylhexacyclo-[6.6.1.1.sup.3,6.1.sup.10,13.0.sup.2,7.0.sup.9,14 
]-4-heptadecene, and 
1,6,10-trimethyl-12-isobutylhexacyclo[6.6.1.1.sup.3,6.1.sup.10,13.0.sup.2,7 
.0.sup.9,14 ]-4-heptadecene: 
Octacyclo[8.8.0.1.sup.2,9.1.sup.4,7.1.sup.11,18.1.sup.13,16.0.sup.3,8.0.sup 
.12,17 ]-5-docosenes; 
octacyclo[8.8.0.1.sup.2,9.1.sup.4,7.1.sup.11,18.1.sup.13,16.0.sup.3,8.0.sup 
.12,17 ]-5-docosene 
##STR5## 
15-methyloctacyclo[8.8.0.1.sup.2,9.1.sup.4,7.1.sup.11,18.1.sup.13,16.0.sup 
. 
3,8.0.sup.12,17 ]-5-docosene, 
15-ethyloctacyclo[8.8.0.1.sup.2,9.1.sup.4,7.1.sup.11,18.1.sup.13,16.0.sup.3 
,8.0.sup.12,17 ]-5-docosene: 
Pentacyclo[6.6.1.1.sup.3,6.0.sup.2,7.0.sup.9,14 ]-4-hexadecenes; 
pentacyclo[6.6.1.1.sup.3,6.0.sup.2,7.0.sup.9,14 ]-4-hexadecene 
##STR6## 
1,3-dimethylpentacyclo[6.6.1.1.sup.3,6.0.sup.2,7.0.sup.9,14 
]-4-hexadecene, 
1,6-dimethylpentacyclo[6.6.1.1.sup.3,6.0.sup.2,7.0.sup.9,14 ]-4-hexadecene, 
15,16-dimethylpentacyclo[6.6.1.1.sup.3,6.0.sup.2,7.0.sup.9,14 
]-4-hexadecene: 
Heptacyclo-5-eicosenes; 
heptacyclo[8.7.0.1.sup.2,9.1.sup.4,7.1.sup.11,17.0.sup.3,8.0.sup.12,16 
]-5-eicosene 
##STR7## 
Heptacyclo-5-heneicosens; 
heptacyclo[8.8.0.1.sup.2,9.1.sup.4,7.1.sup.11,18.0.sup.3,8.0.sup.12,17 
]-5-heneicosene 
##STR8## 
Tricyclo[4.3.0.1.sup.2,5 ]-3-decenes; tricyclo[4.3.0.1.sup.2,5 ]-3-decene 
##STR9## 
2-methyltricyclo[4.3.0.1.sup.2,5 ]-3-decene, 
5-methyltricyclo[4.3.0.1.sup.2,5 ]-3-decene: 
Tricyclo[4.4.0.1.sup.2,5 ]-3-undecenes; 
tricyclo[4.4.0.1.sup.2,5 ]-3-undecene 
##STR10## 
10-methyl-tricyclo[4.4.0.1.sup.2,5 ]-3-undecene: 
Pentacyclo[6.5.1.1.sup.3,6.0.sup.2,7.0.sup.9,13 ]-4-pentadecenes; 
pentacyclo[6.5.1.1.sup.3,6.0.sup.2,7.0.sup.9,13 ]-4-pentadecene 
##STR11## 
1,3-dimethyl-pentacyclo[6.5.1.1.sup.3,6.0.sup.2,7.0.sup.9,13 
]-4-pentadecene, 
1,6-dimethylpentacyclo[6.5.1.1.sup.3,6.0.sup.2,7.0.sup.9,13 
]-4-pentadecene, 
14,15-dimethylpentacyclo[6.5.1.1.sup.3,6.0.sup.2,7.0.sup.9,13 
]-4-pentadecene: 
Pentacyclopentadecadienes; 
pentacyclo[6.5.1.1.sup.3,6.0.sup.2,7.0.sup.9,13 ]-4,10-pentadecadiene 
##STR12## 
Pentacyclo[4.7.0.1.sup.2,5.0.sup.8.13.1.sup.9,12 ]-3-pentadecenes; 
pentacyclo[4.7.0.1.sup.2,5.0.sup.8.13.1.sup.9,12 ]-3-pentadecene 
##STR13## 
methyl-substituted pentacyclo[4.7.0.1.sup.2,5.0.sup.8.13.1.sup.9,12 
]-3-pentadecene: 
Heptacyclo[7.8.0.1.sup.3,6.0.sup.2,7.1.sup.10,17.0.sup.11,16.1.sup.12,15 
]-4-eicosenes; 
heptacyclo[7.8.0.1.sup.3,6.0.sup.2,7.1.sup.10,17.0.sup.11,16.1.sup.12,15 
]-4-eicosene 
##STR14## 
dimethyl-substituted 
heptacyclo[7.8.0.1.sup.3,6.0.sup.2,7.1.sup.10,17.0.sup.11,16.1.sup.12,15 
]-4-eicosene: 
Nonacyclo[9.10.1.1..sup.4.7.0.sup.3,8.0.sup.2,10.0.sup.12,21.1.sup.13,20.0. 
sup.14,19.1.sup.15,18 ]-5-pentacosenes; 
nonacyclo[9.10.1.1..sup.4.7.0.sup.3,8.0.sup.2,10.0.sup.12,21.1.sup.13,20.0. 
sup.14,19.1.sup.15,18 ]-5-pentacosene 
##STR15## 
trimethyl-substituted 
nonacyclo[9.10.1.1..sup.4.7.0.sup.3,8.0.sup.2,10.0.sup.12,21.1.sup.13,20.0 
.sup.14,19.1.sup.15,18 ]-5-pentacosene: 
Pentacyclo[4.8.4.sup.2,5.0.sup.8,13.1.sup.9,12 ]-3-hexadecenes; 
pentacyclo[4.8.4.sup.2,5.0.sup.8,13.1.sup.9,12 ]-3-hexadecene 
##STR16## 
10-methyl-pentacyclo[4.8.4.sup.2,5.0.sup.8,13.1.sup.9,12 ]-3-hexadecene, 
10-ethyl-pentacyclo[4.8.4.sup.2,5.0.sup.8,13.1.sup.9,12 ]-3-hexadecene, 
10,11-dimethyl-pentacyclo[4.8.4.sup.2,5.0.sup.8,13.1.sup.9,12 
]-3-hexadecene: 
Heptacyclo[8.8.0.0.sup.3,8.1.sup.4,7.1.sup.11,18.0.sup.12,17.1.sup.13,16 
]-5-heneicosenes; 
heptacyclo[8.8.0.0.sup.3,8.1.sup.4,7.1.sup.11,18.0.sup.12,17.1.sup.13,16 
]-5-heneicosene 
##STR17## 
14-methyl-heptacyclo[8.8.0.0.sup.3,8.1.sup.4,7.1.sup.11,18.0.sup.12,17.1.su 
p.13,16 ]-5-heneicosene, 
trimethyl-heptacyclo[8.8.0.0.sup.3,8.1.sup.4,7.1.sup.11,18.0.sup.12,17.1.su 
p.13,16 ]-5-heneicosene: 
Nonacyclo[10.10.1.0.sup.2,11.0.sup.4,9.1.sup.5,8.0.sup.13,22.1.sup.14,21.0. 
sup.15,20.1.sup.16,19 ]-6-hexacosenes; 
nonacyclo[10.10.1.0.sup.2,11.0.sup.4,9.1.sup.5,8.0.sup.13,22.1.sup.14,21.0. 
sup.15,20.1.sup.16,19 ]-6-hexacosene 
##STR18## 
The cycloolefin/ethylene random copolymer (a4) can be obtained by 
copolymerizing a cycloolefin of the above formula (I), ethylene and 
optionally, other olefin compound. 
The other olefin compound copolymerizable with ethylene and the cycloolefin 
compound of the above formula (I) in the present invention is selected 
from .alpha.-olefins having 3 to 20 carbon atoms such as propylene, 
1-butene, 4-methyl-1-pentene, 1-hexene, 1-octene, 1-decene, 1-dodecene, 
1-tetradecene, 1-hexadecene, 1-octadecene, and 1-eicosene; 
cycloolefins such as cyclopentene, cyclohexene, 3-methylcyclohexene, 
cyclooctene, and 3a,5,6,7a-tetrahydro-4,7-methano-1H-indene; 
conjugated dienes such as 1,4-hexadiene, 4-methyl-1,4-hexadiene, 
5-methyl-1,4-hexadiene, 1,7-octadiene, dicyclopentadiene, 
5-ethylidene-2-norbornene, and 5-vinyl-2-norbornene; and 
norbornenes such as norbornene-2, 5-methylnorbornene-2, 
5-ethylnorbornene-2, 5-isopropylnorbornene-2, 5-n-butylnorbornene-2, 
5-i-butylnorbornene-2, 5,6-dimethylnorbornene-2, 5-chloronorbornene-2, 
2-fluoronorbornene-2, and 5,6-dichloronorbornene-2. 
The above "other olefin" is used in an amount, based on the total amount of 
the cycloolefin, ethylene and this other olefin, of preferably not more 
than about 20 mol %, more preferably not more than 10 mol %. 
The above reaction of ethylene, the cycloolefin of the formula (I) and 
optionally other olefin is generally carried out in a hydrocarbon solvent. 
The hydrocarbon solvent used in this reaction is selected, for example, 
from aliphatic hydrocarbons such as hexane, heptane, octane and kerosene; 
alicyclic hydrocarbons such as cyclohexane and methylcyclohexane; and 
aromatic hydrocarbons such as benzene, toluene and xylene. Further, 
polymerizable unsaturated monomers which can be used for the preparation 
of the cycloolefin random copolymer and which are liquid compounds at a 
reaction temperature may be used as a reaction solvent. These solvents may 
be used alone or in combination. 
The catalyst used for the reaction of the above olefin with the cycloolefin 
of the formula (I) is selected from catalysts comprising vanadium 
compounds soluble in a hydrocarbon solvent used as a reaction solvent and 
organoaluminum compounds. 
Examples of the vanadium compounds used as a catalyst are compounds of the 
formula, VO(OR).sub.a V.sub.b or the formula, V(OR).sub.c X.sub.d. 
In the above formulae, R is a hydrocarbon group, and there are relations of 
0.ltoreq.a.ltoreq.3, 0.ltoreq.b.ltoreq.3, 2.ltoreq.a+b.ltoreq.3, 
0.ltoreq.c.ltoreq.4, 0.ltoreq.d.ltoreq.4 and 3.ltoreq.c+d.ltoreq.4. 
Further, the vanadium compounds may be adducts of vanadium compounds of the 
above formulae with electron donors. 
Examples of the above vanadium compounds are: 
VOCl.sub.3, 
VO(OC.sub.2 H.sub.5)Cl.sub.2, 
VO(OC.sub.2 H.sub.5).sub.2 Cl, 
VO(O--iso--C.sub.3 H.sub.7)Cl.sub.2, 
VO(O--n--C.sub.4 H.sub.9)Cl.sub.2, 
VO(OC.sub.2 H.sub.5).sub.3, 
VOBr.sub.2, 
VCl.sub.4, 
VOCl.sub.2, 
VO(O--n--C.sub.4 H.sub.9).sub.3, and 
VCl.sub.3.2(OC.sub.8 H.sub.17 OH). 
These vanadium compounds may be used alone or in combination. 
Examples of the electron donors which form adducts with the above vanadium 
compounds are oxygen-containing electron donors such as alcohol, phenols, 
ketone, aldehyde, carboxylic acid, organic or inorganic acid ester, ether, 
acid amide, acid anhydride, and alkoxysilane, and nitrogen-containing 
electron donors such as ammonia, amine, nitrile and isocyanate. 
Specific compound usable as such an electron donor is selected from: 
alcohols having 1 to 18 carbon atoms such as methanol, ethanol, propanol, 
pentanol, hexanol, octanol, dodecanol, octadecyl alcohol, oleyl alcohol, 
benzyl alcohol, phenyl ethyl alcohol, cumyl alcohol, isopropyl alcohol, 
and isopropylbenzyl alcohol; 
phenols having 6 to 20 carbon atoms such as phenol, cresol, xylenol, 
ethylphenol, propylphenol, nonylphenyl, cumylphenol, and naphthol (these 
phenols may have a lower alkyl group); 
ketones having 3 to 15 carbon atoms such as acetone, methyl ethyl ketone, 
methyl isobutyl ketone, acetophenone, benzophenone, and benzoquinone; 
aldehydes having 2 to 15 carbon atoms such as acetaldehyde, 
propionaldehyde, octylaldehyde, benzaldehyde, tolualdehyde, and 
naphthoaldehyde; 
organic acid esters having 2 to 30 carbon atoms such as methyl formate, 
methyl acetate, ethyl acetate, vinyl acetate, propyl acetate, octyl 
acetate, cyclohexyl acetate, ethyl propionate, methyl butyrate, ethyl 
valerate, methyl chloroacetate, ethyl dichloroacetate, methyl 
methacrylate, ethyl crotonate, ethyl cyclohexanecarboxylate, methyl 
benzoate, ethyl benzoate, propyl benzoate, butyl benzoate, octyl benzoate, 
cyclohexyl benzoate, phenyl benzoate, benzyl benzoate, methyl toluylate, 
ethyl toluylate, amyl toluylate, ethyl ethylbenzoate, methyl anisate, 
n-butyl maleate, diisobutyl methylmalonate, di-n-hexyl 
cyclohexenecarboxylate, diethyl Nadic acid ester, diisopropyl 
tetrahydrophthalate, diethyl phthalate, di-n-butyl phthalate, 
di-2-ethylhexyl phthalate, .gamma.-butyrolactone, .delta.-valerolactone, 
coumarin, phthalide, and ethylene carbonate; 
acid halides having 2 to 15 carbon atoms such as acetyl chloride, benzoyl 
chloride, toluic acid chloride, and anisic acid chloride; 
ethers having 2 to 20 carbon atoms such as methyl ether, ethyl ether, 
isopropyl ether, butyl ether, amyl ether, tetrahydrofuran, anisole, and 
diphenyl ether; 
acid amides such as acetic amide, benzoic amide, and toluic amide, 
amines such as methylamine, ethylamine, diethylamine, tributylamine, 
piperidine, tribenzylamine, aniline, pyridine, picoline, and 
tetramethylenediamine; 
nitriles such as acetonitrile, benzonitrile, and tolunitrile; and 
alkoxysilanes such as ethyl silicate and diphenyldimethoxysilane. These 
electron donors may be used alone or in combination. 
The organoaluminum compounds usable in the above reaction have at least one 
Al-carbon bond in the molecule. 
Examples of the organoaluminum compounds used above are: 
(i) organoaluminum compounds of the formula, R.sup.21.sub.e 
Al(OR.sup.22).sub.f H.sub.g X.sub.h, 
(wherein each of R.sup.21 and R.sup.22 is, independently of the other, a 
hydrocarbon group which generally has 1 to 15 carbon atoms, preferably has 
1 to 4 carbon atoms, X is a halogen, e is defined by 0.ltoreq.e.ltoreq.3, 
f is defined by 0.ltoreq.f&lt;3, g is defined by 0.ltoreq.g&lt;3, h is defined 
by 0.ltoreq.h&lt;3, and e+f+g+h=3), and 
(ii) alkylation product complexes of a Group 1 metal and aluminum, of the 
formula, M.sup.1 AlR.sup.21.sub.4, 
(wherein M.sup.1 is Li, Na or K and R.sup.21 is as defined above). 
Specific examples of the organoaluminum compounds of the above formula (i) 
are as follows. 
Compounds of the formula, R.sup.21.sub.i Al(OR.sup.22).sub.3-i, 
(wherein R.sup.21 and R.sup.22 are as defined above, and i is preferably a 
number defined by 1.5.ltoreq.i&lt;3). 
Compounds of the formula, R.sup.21.sub.e AlX.sub.3-e, 
(wherein R.sup.21 is as defined above, X is a halogen, e is preferably 
defined by 0&lt;e&lt;3). 
Compounds of the formula, R.sup.21.sub.j AlH.sub.3-j, 
(wherein R.sup.21 is as defined above, and j is preferably defined by 
2.ltoreq.j&lt;3). 
Compounds of the formula, R.sup.21.sub.e Al(OR.sup.22).sub.f X.sub.h, 
(wherein R.sup.21 and R.sup.22 are as defined above, X is a halogen, 
0&lt;e.ltoreq.3, 0.ltoreq.f&lt;3, 0.ltoreq.h&lt;3, and e+f+H=3). 
Specific examples of the organoaluminum compounds of the above formula (II) 
are: 
trialkylaluminum such as triethylaluminum and tributylaluminum; 
trialkylaluminum such as triisopropylaluminum, 
dialkylaluminum alkoxides such as diethylaluminum ethoxide, and 
dibutylaluminum butoxide; 
alkylaluminum sesquialkoxides such as ethylaluminum sesquiethoxide, and 
butylaluminum sesquibutoxide; 
partially alkoxylated alkylaluminum having an average composition of the 
formula, R.sup.21.sub.2.5 Al(OR.sup.22).sub.0.5, etc; 
dialkylaluminum halides such as diethylaluminum chloride, dibutylaluminum 
chloride, and diethylaluminum bromide; 
alkylaluminum sesquihalides such as ethylaluminum sesquichloride, 
butylaluminum sesquichloride, and ethylaluminum sesquibromide; 
partially halogenated alkylaluminum such as ethylaluminum dichloride, 
propylaluminum dichloride, and butylaluminum dibromide; 
dialkylaluminum hydrides such as diethylaluminum hydride and 
dibutylaluminum hydride; 
partially hydrogenated alkylaluminum such as alkylaluminum dihydrides, 
e.g., ethylaluminum dihydride and propylaluminum dihydride; and 
partially alkoxylated and halogenated alkylaluminum such as ethylaluminum 
ethoxychloride, butylaluminum butoxychloride, and ethylaluminum 
ethoxybromide. 
The organoaluminum compound may also be a compound similar to the compounds 
of the formula (ii) such as aluminum compounds in which two or more 
aluminum atoms are bonded through an oxygen atom or a nitrogen atom. 
Specific examples of such a compound are: 
##STR19## 
Examples of the organoaluminum compounds of the formula (ii) are: 
EQU LiAl(C.sub.2 H.sub.5).sub.4 
EQU and 
EQU LiAl(C.sub.7 H.sub.15).sub.4. 
of these, it is preferred to use alkylaluminum halide, alkylaluminum 
dihalide or a mixture of these. 
The amount, as a vanadium atom, of the above vanadium compound for use is 
generally in the range of 0.01 to 5 gram-atom/lit., preferably in the 
range of 0.05 to 3 gram-atom/lit. The amount of the organoaluminum 
compound, as a ratio of an aluminum atom to a vanadium atom (Al/V) in a 
polymerization reaction system, is generally not less than 2, preferably 2 
to 50, particularly preferably 3 to 20. 
The cycloolefin-based polymer (a) obtained in the presence of the above 
catalyst contains preferably 52 to 90 mol %, more preferably 55 to 80 mol 
% of an ethylene component unit, and it contains preferably 10 to 48 mol 
%, more preferably 20 to 45 mol % of a recurring unit derived from the 
cycloolefin. In addition, when the cycloolefin-based polymer (a) contains 
an olefin component unit other than the ethylene component unit, the 
content of this olefin component unit in the cycloolefin-based polymer is 
preferably not more than 20 mol %, more preferably not more than 10 mol %. 
In the cycloolefin-based polymer (a) used in the present invention, the 
ethylene component unit and the recurring one derived from the cycloolefin 
are substantially linearly arranged, and further these recurring units are 
arranged at random. 
In the cycloolefin-based polymer (a) used in the present invention, the 
recurring unit which constitutes the alicyclic structure has a structure 
of the following formula (II), 
##STR20## 
wherein R.sup.1 to R.sup.18, n, m and q are as defined in the above 
formula (I). 
The above cycloolefin-based polymer is incorporated in an amount in the 
range of 50 to 95 parts by weight per 100 parts by weight of the total 
amount of the component (a), the component (b) and the component (c). In 
particular, it is preferred to adjust this amount to the range of 60 to 85 
parts by weight. 
When the component (a) is incorporated in the above amount, there can be 
obtained a resin composition which is improved in mechanical properties 
such as impact strength, etc., without impairing excellent properties of 
the cycloolefin-based polymer (a). 
The graft-modified elastomer (b) used in the present invention is an 
elastomer which is obtained by graft-modification with an unsaturated 
carboxylic acid or a derivative thereof and has a tensile modulus, at 
23.degree. C., of 0.1 to 2,000 kg/cm.sup.2. The tensile modulus is 
preferably in the range of 1 to 1,500 kg/cm.sup.2. The glass transition 
temperature (Tg) of this graft-modified elastomer is preferably in the 
range of -150.degree. to +50.degree. C., more preferably in the range of 
-80.degree. to -20.degree. C. The intrinsic viscosity [.eta.], measured in 
decalin at 135.degree. C., of this graft-modified elastomer is preferably 
0.2 to 10 dl/g, more preferably 1 to 5 dl/g. The density thereof is 
preferably 0.82 to 0.96 g/cm.sup.3, more preferably 0.84 to 0.92 
g/cm.sup.3. Further, the crystallinity, measured by an X-ray diffraction 
method, of this graft-modified elastomer is preferably not more than 30%, 
more preferably not more than 25%. 
When the graft-modified elastomer (b) used in the present invention is a 
graft-modified .alpha.-olefin copolymer, specific examples of the 
graft-modified .alpha.-olefin copolymer are: 
(i) graft-modified ethylene..alpha.-olefin copolymer rubber, and 
(ii) graft-modified propylene..alpha.-olefin copolymer rubber. The above 
graft-modified ethylene..alpha.-olefin copolymer rubber (i) and 
graft-modified propylene..alpha.-olefin copolymer rubber (ii) may be used 
alone or in combination. 
The .alpha.-olefin to constitute the above graft-modified 
ethylene..alpha.-olefin copolymer rubber (i) is generally selected from 
.alpha.-olefins having 3 to 20 carbon atoms such as propylene, 1-butene, 
1-pentene, 1-hexene, 4-methyl-1-pentene, 1-octene, 1-decene and mixtures 
of these. Of these, particularly preferred are propylene and/or 1-butene. 
The .alpha.-olefin to constitute the graft-modified 
propylene..alpha.-olefin copolymer rubber (ii) is generally selected from 
.alpha.-olefins having 4 to 20 carbon atoms such as 1-butene, 1-pentene, 
1-hexene, 4-methyl-1-pentene, 1-octene, 1-decene and mixtures of these. Of 
these, particularly preferred is 1-butene. 
In addition, the .alpha.-olefin copolymer used in the present invention may 
contain a component unit other than the unit derived from the 
.alpha.-olefin, such as a component unit derived from a diene compound, in 
such an amount that does not impair the properties of the .alpha.-olefin 
copolymer. 
Examples of the component unit which may be contained in the .alpha.-olefin 
copolymer used in the present invention are linear non-conjugated dienes 
such as 1,4-hexadiene, 1,6-octadiene, 2-methyl-1,5-hexadiene, 
6-methyl-1,5-heptadiene, and 7-methyl-1,6-octadiene; 
cyclic non-conjugated dienes such as cyclohexadiene, dicyclopentadiene, 
methyltetrahydroindene, 5-vinylnorbornene, 5-ethylidene-2-norbornene, 
5-methylene-2-norbornene, 5-isopropylidene-2-norbornene, and 
6-chloromethyl-5-isopropenyl-2-norbornene; 
components units derived from diene compounds such as 
2,3-diisopropylidene-5-norbornene, 
2-ethylidene-3-isopropylidene-5-norbornene, and 
2-propenyl-2,2-norbornadiene; and 
the above cycloolefin components. The content of the above diene component 
is preferably not more than 10 mol %, more preferably not more than 5 mol 
%. 
In the graft-modified ethylene..alpha.-olefin copolymer (i) used in the 
present invention, although differing depending upon the kind of the 
.alpha.-olefin, the molar ratio of ethylene to the .alpha.-olefin 
(ethylene/.alpha.-olefin) is preferably 10/90 to 90/10, more preferably 
50/50 to 90/10. When the .alpha.-olefin is propylene, the above molar 
ratio is preferably 50/50 to 90/10. When the .alpha.-olefin is an 
.alpha.-olefin having 4 or more carbon atoms, the above molar ratio is 
preferably 50/50 to 90/10. 
In the graft-modified propylene..alpha.-olefin copolymer (ii) used in the 
present invention, although differing depending upon the kind of the 
.alpha.-olefin, the molar ratio of propylene to the .alpha.-olefin 
(propylene/.alpha.-olefin) is, in general, preferably 50/50 to 90/10. When 
the .alpha.-olefin is 1-butene, the above molar ratio is preferably 50/50 
to 90/10. When the .alpha.-olefin is an .alpha.-olefin having 5 or more 
carbon atoms, it is preferably 50/50 to 90/10. 
In the present invention, it is preferred to select, out of the above 
graft-modified elastomers (b), a copolymer obtained by graft-modification 
of an ethylene propylene random copolymer or ethylene..alpha.-olefin 
random copolymer having an ethylene content of 35 to 50 mol % and a 
crystallinity of not more than 10% with a graft monomer, since such a 
copolymer has an excellent effect on improvement of mechanical properties 
such as impact strength. 
The graft monomer used for the preparation of the graft-modified elastomer 
(b) used in the present invention is selected from unsaturated carboxylic 
acids or derivatives thereof. Examples of the unsaturated carboxylic acid 
are acrylic acid, maleic acid, fumaric acid, tetrahydrophthalic acid, 
itaconic acid, citraconic acid, crotonic acid, isocrotonic acid, and Nadic 
acid.RTM. (endo-cis-bicyclo[2,2,1]hept-5-ene-2,3-dicarboxylic acid). 
Examples of the derivatives of the above unsaturated carboxylic acid are 
unsaturated carboxylic acid anhydrides, unsaturated carboxylic acid 
halides, unsaturated carboxylic acid amides, unsaturated carboxylic acid 
imides and ester compounds of unsaturated carboxylic acids. Specific 
examples of these derivatives are malenyl chloride, maleimide, maleic 
anhydride, citraconic anhydride, monomethyl maleate, dimethyl maleate, 
glycidyl meleate, glycidyl acrylate, and glycidyl methacrylate. 
These graft monomers may be used alone or in combination. 
Of the above graft monomers, preferred are unsaturated carboxylic acids or 
anhydrides thereof, and particularly preferred are maleic acid, Nadic 
acid.RTM. and anhydrides of these or glycidyl methacrylate and glycidyl 
acrylate. 
The graft-modified elastomer (b) used in the present invention can be 
prepared, for example, by modifying the .alpha.-olefin copolymer with the 
above graft monomer by any one of various known methods. For example, 
there is available a method in which the above .alpha.-olefin copolymer is 
melted and the graft monomer is added thereto for graft polymerization, or 
a method in which the graft monomer dissolved in a solvent is added for 
graft polymerization. Further, the graft-modified elastomer can be also 
prepared by other method in which the graft monomer is incorporated into 
an unmodified .alpha.-olefin copolymer such that the .alpha.-olefin 
copolymer has a desired graft modification ratio, or in which a 
graft-modified .alpha.-olefin having a high graft modification ratio is 
prelimiarily prepared and this .alpha.-olefin copolymer having a high 
graft modification ratio is diluted with an unmodified .alpha.-olefin 
copolymer to prepare a graft-modified elastomer having a desired 
modification ratio. In the present invention, a graft-modified elastomer 
prepared by any one of the above methods may be used. The graft-modified 
elastomer (b) used in the present invention is a copolymer having a graft 
modification ratio in the range of preferably 0.01 to 5% by weight, more 
preferably 0.1 to 4% by weight. 
The above reaction is carried out preferably in the presence of a radical 
initiator in order to effectively carry out the graft copolymerization 
with the above graft monomer. The graft reaction is generally carried out 
at a temperature between 60.degree. C. and 350.degree. C. The amount of 
the radical initiator for use is generally in the range of 0.001 to 5 
parts by weight per 100 parts by weight of the unmodified .alpha.-olefin 
elastomeric copolymer. 
As the radical initiator, organic peroxides and organic peresters can be 
preferably used. Specific examples of these radical initiators are benzoyl 
peroxide, dichlorobenzoyl peroxide, dicumyl peroxide, di-tert-butyl 
peroxide, 2,5-dimethyl-2,5-di(peroxidebenzoate)hexyne-3, 
1,4-bis(tert-butylperoxyisopropyl)benzene, lauroyl peroxide, tertbutyl 
peracetate, 2,5-dimethyl-2,5-di(tert-butylperoxy)hexyne-3, 
2,5-dimethyl-2,5-di(tert-butyloxy)hexane, tert-butyl perbenzoate, 
tert-butylperphenyl acetate, tert-butyl perisobutylate, tert-butyl 
per-sec-octoate, tert-butyl perpivalate, cumyl perpivalate, and tert-butyl 
perdiethylacetate. In the present invention, further, an azo compound may 
be used as a radical initiator. Specific examples of the azo compound are 
azobisisobutyronitrile and dimethylazoisobutyrate. 
Of these, preferred as the radical initiator are dialkyl peroxides such as 
benzoyl peroxide, dicumyl peroxide, di-tert-butyl peroxide, 
2,5-dimethyl-2,5-di(tert-butylperoxy)hexyne-3, 
2,5-dimethyl-2,5-di(tert-butylperoxy)hexane and 
1,4-bis(tert-butylperoxyisopropyl)benzene. 
As the graft-modified elastomer (b) used in the present invention, the 
above graft-modified ethylene..alpha.-olefin copolymer (i) and the above 
graft-modified propylene..alpha.-olefin copolymer (ii) are generally used 
alone or in combination. However, other polymer, copolymer or graft 
copolymer may be used in combination in such an amount that does not 
impair the properties of the graft-modified elastomer. 
Examples of the above "other polymer or copolymer" in the present invention 
are aromatic vinyl-containing hydrocarbon.conjugated diene copolymers or 
hydrides thereof. Specific examples of the aromatic vinyl-containing 
hydrocarbon.conjugated diene copolymers or the hydrides thereof are 
styrene.butadiene copolymer rubber, styrene.butadiene.styrene copolymer 
rubber, styrene.isoprene block copolymer rubber, styrene.isoprene.styrene 
block copolymer rubber, hydrogenated styrene.butadiene.styrene block 
copolymer rubber and hydrogenated styrene.isoprene.styrene block copolymer 
rubber. 
The above graft-modified elastomer (b) is incorporated in an amount in the 
range of 1 to 50 parts by weight per 100 parts by weight of the total 
amount of the component (a), the component (b) and the component (c). It 
is particularly preferred to adjust this amount to the range of 10 to 30 
parts by weight. 
When the component (b) in the above amount is incorporated, there can be 
obtained a resin composition which is improved in mechanical properties 
such as impact strength without impairing excellent properties of the 
cycloolefin-based polymer (a). 
The polyolefin resin composition of the present invention contains, as a 
component (c), a compound having one amino group in the molecule. The 
concept of "compound" used here includes a condensate, a ring-opening 
reaction product and a high-molecular-weight compound. 
In the present invention, the following compounds are suitably usable as a 
component (c). 
(C1) a condensate having one amino group in the molecule. 
(C2) a ring-opening reaction product having one amino group in the 
molecule. 
(C3) a polymer in which one amino group is bonded to a polyolefin having a 
molecular weight of not less than 20,000. 
(C4) a low-molecular-weight amino compound in which one of the molecule 
terminals is an amino group. 
That is, the condensate (C1) used as a component (c) in the present 
invention is a product formed by a condensation reaction, and refers 
mainly to an oligomer or polymer of an aminocarboxylic acid. The 
ring-opening reaction product (C2) is a product formed by a ring-opening 
reaction and refers mainly to a ring-opening polymerization polymer from 
lactams. Further, the polymer (C3) is a polymer in which one amino group 
is bonded to a polyolefin having a molecular weight of not less than 
20,000. The low-molecular-weight amino compound (C4) having one amino 
group in the molecule refers mainly to a monomer used for the preparation 
of the above condensate (C1) or the above ring-opening reaction product 
(C2). 
In the present invention, as a component (c), the component (C1), the 
component (C2), the component (C3) and the component (C4) may be used 
alone or as a mixture of at least two of these. 
In the present invention, as a compound which is particularly effective as 
the low-molecular-weight amino compound (C-4) in which one of the molecule 
terminals is an amino group, used as a component (c), there is a compound 
of the following formula (C4a) or (C4b). 
##STR21## 
In the above formulae (C4a) and (C4b), R.sup.23 is an alkylene group. 
Specific examples of the above low-molecular-weight amino compound are 
.epsilon.-aminocaproic acid, 7-aminoheptanoic acid, 
.omega.-aminoundecanoic acid, laurolactam, .omega.-aminononanoic acid, 
.beta.-propiolactam, 2-piperidone, .gamma.-butyrolactam, 
11-aminoundecanoic acid, .alpha.-pyrropydone, .gamma.-aminobutyric acid, 
.beta.-alanine, 8-aminovaleric acid, and .epsilon.-aminolactam. 
Examples of the amino group-containing condensate (C1) or the ring-opening 
reaction product (C2) are preferably compounds or ring-opening 
polymerization polymers (or polycondensation polymers) formed by 
condensation reactions of compounds containing an amino group and a 
carboxyl group, which can have (or have) an amino group and a carboxyl 
group, such as an aminocarboxylic acid, or a dicarboxylic acid with a 
diamine, or .epsilon.-aminocaprolactam, or functional derivatives thereof. 
Typical examples of the amino group-containing condensate (C1) are 
polyamide precursors and polyamide resins. Examples of the polyamide 
precursors are aliphatic amines such as ethylenediamine, propylenediamine, 
hexamethylenediamine, diethylenetriamine, triethylenetetramine, 
tetraethylenepentamine, iminobispropylamine, bis(hexamethylene)triamine, 
1,3,6-trisaminomethylhexane, trimethylhexamethylenediamine, 
bispropylenediamine, and diethylaminopropylamine; 
alicyclic amines such as menthenediamine, isophoronediamine, 
bis(4-amino-3-methylcyclohexyl)methane, N-aminoethylpiperazine, and 
1,3-diaminocyclohexane; 
aliphatic aromatic amines such as m-xylylenediamine; 
aromatic amines such as o-, m- or p-phenylenediamine, 
diaminodiphenylmethane, diaminodiphenylsulfone, 2,4-diaminoanisole, 
2,4-toluenediamine, 2,4-diaminidiphenylamine, 4,4'-methylenedianiline, and 
diaminodixylylsulfone; 
oligomers formed by polycondensation of diamine components such as 
bisspiro-cyclized diamines, e.g., 
3,9-bis(3-aminopropyl)-2,4,8,10-tetraspiro[5,5]undecane with dicarboxylic 
acids such as adipic acid, sebacic acid, terephthalic acid, isophthalic 
acid, dodecanoic diacid, and glutaric acid; and 
oligomers formed by ring-opening polymerization or polycondensation of 
.epsilon.-caprolactam, aminocaproic acid, enantholactam, 7-aminoheptanoic 
acid, and 11-aminoundecanoic acid. 
In the present invention, the "oligomer" refers to the above condensate or 
ring-opening polymerization product having a molecular weight of less than 
2,000. 
Examples of the polyamide resins are those which are condensates of the 
above diamine components and either the above dicarboxylic acid components 
or .epsilon.-aminoundecanoic acid and ring-opening polymerization polymers 
of the above lactams and have a molecular weight of not less than 2,000. 
Specific examples thereof are nylon-2, nylon-3, nylon-4, nylon-5, nylon-6, 
nylon-7, nylon-8, nylon-9, nylon-10, nylon-11, nylon-12, nylon-13, 
nylon-66, nylon-610, nylon-612, copolymer nylon formed from caprolactam 
and a nylon salt aqueous solution, nylon MXD6 formed from 
m-xylylenediamine and adipic acid, nylon-46, and methoxymethylated 
polyamide. 
In the present invention, the above oligomers and polyamides may be used 
alone or in combination. 
Of these, preferred are polyamide resins which have an amino group on one 
terminal and are crystalline, such as nylon 6, nylon 11 and nylon 12. 
The polymer (C3) in which one amino group is bonded to a polyolefin having 
a molecular weight of not less than 20,000 refers, for example, to a 
polymer in which one amino group is bonded to a polymer of an 
.alpha.-olefin such as ethylene or propylene. Such a polymer (C3) can be 
prepared by introducing an amino group to a polyolefin according to a 
known method. 
The above compound (c) having an amino group is incorporated in an amount 
of 0.01 to 45 parts by weight per 100 parts by weight of the total amount 
of the component (a), the component (b) and the component (c). It is 
particularly preferred to adjust this amount to the range of 0.01 to 30 
parts by weight. 
Owing to the incorporation of the compound (c) having an amino group, there 
can be formed a molded article which is excellent particularly in impact 
strength and gloss. That is, these components (C1), (C2) and (C3) has 
relatively high crystallinity around room temperature, and due to this 
crystallinity, the cycloolefin-based resin is improved in properties. The 
component (C4) in the composition also works in the same way as the 
components (C1), (C2) and (C3). It is considered that when by 
incorporation of this compound (c) having an amino group, the compound (c) 
exhibits a reinforcing effect since its crystal has an effect similar to 
that of a crosslinking agent at a temperature not higher than the melting 
point of this compound to form a crosslinked structure-like structure in 
the graft-modified copolymer, and that the composition exhibits excellent 
moldability since with an increase in temperature, the reinforcing effect 
due to the structure similar to a crosslinked structure decreases and the 
composition gradually has excellent flowability. 
In addition to the above components, the polyolefin resin composition of 
the present invention may contain additives such as an inorganic filler, 
an organic filler, a thermal stabilizer, a weathering stabilizer, an 
antistatic agent, an anti-slipping agent, an antiblocking agent, an 
anti-fogging agent, a lubricant, a pigment, a dye, natural oil, synthetic 
oil, wax, etc. 
The polyolefin resin composition of the present invention can be produced, 
for example, by a method in which the cycloolefin-based polymer (a) and 
the graft-modified elastomer (b) are separately prepared, a mixture of 
these cycloolefin-based polymer and graft-modified elastomer (b) are 
melt-kneaded, further, the compound (c) having an amino group is 
incorporated into the kneaded mixture and further kneaded; by a method in 
which the cycloolefin-based polymer (a), the graft-modified elastomer (b) 
and the compound (c) having an amino group are melt-kneaded at one lot; 
and particularly by a method in which the graft-modified elastomer (b) and 
the compound (c) having an amino group are melt-kneaded, the resultant 
kneaded mixture is incorporated into the cycloolefin-based polymer (a) and 
further kneaded. 
The above polyolefin resin composition containing the cycloolefin-based 
polymer (a), the graft-modified elastomer (b) and the compound (c) having 
an amino group, provided by the present invention, has a softening 
temperature (TMA), measured with a thermal mechanical analyzer, of 
generally between 50.degree. C. and 200.degree. C., preferably between 
100.degree. C. and 180.degree. C. 
The polyolefin resin composition of the present invention can be used not 
only in fields where ordinary polyolefins are used but also in fields 
where, for example, filler-reinforced PP, ABS resin and modified 
polyphenylene oxide are used and mechanical strength is particularly 
required. 
The polyolefin resin composition of the present invention has a structure 
in which the graft-modified elastomer (b) is dispersed in the 
cycloolefin-based polymer (a). And it is considered that due to the 
incorporation of the compound (c) having an amino group, a structure 
similar to a crosslinked structure is formed in the interior of the 
graft-modified elastomer (b). A molded article formed of such a polyolefin 
resin composition has excellent impact strength. In particular, due to the 
use of the compound having an amino group in the molecule, the 
contribution of the structure similar to a crosslinked structure decreases 
when the polyolefin resin composition is melted. As a result, such a 
polyolefin resin composition exhibits excellent flowability, and moreover, 
a molded article therefrom has excellent impact strength and gloss.

The present invention will be described below by reference to Examples. 
However, Examples shall not be construed as limitations to the present 
invention. 
EVALUATION METHOD 
Cycloolefin-based polymers, graft-modified elastomers and compounds having 
an amino group, used in the present invention, and polyolefin resin 
compositions of the present invention were measured for their properties 
as follows. 
INTRINSIC VISCOSITY [.eta.] 
Measured in decalin at 135.degree. C. 
SOFTENING TEMPERATURE (TMA) 
A temperature at which a needle having a diameter of 1 mm and a flat end 
penetrates 100 .mu.m deep at a temperature elevation rate of 5.degree. 
C./minute under a load of 50 g was taken as a TMA. 
CONTENT OF GRAFT MONOMER IN GRAFT-MODIFIED ELASTOMER 
Measured by .sup.13 C-NMR. 
CRYSTALLINITY 
Measured at 23.degree. C. by an X-ray diffraction method. 
TENSILE MODULUS 
A press-formed test piece having a thickness of 2 mm was measured at 
23.degree. C. according to ASTM D638. 
IZ IMT STRENGTH 
A notched, injection-molded test piece having a thickness of 1/8 inch was 
measured at 23.degree. C. according to ASTM D256. 
INITIAL FLEXURAL MODULUS (FM) 
An injection-molded test piece having a thickness of 1/8 inch was measured 
at a cross head speed of 20 mm/minute at 23.degree. C. according to ASTM 
D790. 
FLEXURAL STRESS AT YIELD POINT (FS) 
Measured in the same manner as in the measurement for FM according to ASTM 
D790. 
GLOSS 
An injection-molded plate having a thickness of 2 mm was measured at an 
incident angle of 60 degrees at 23.degree. C. according to ASTM D523. 
MELT INDEX (MI) 
Measured at 260.degree. C. under a load of 2.16 kg according to JIS-K-6760. 
PREATION EXAMPLE 1 
Preparation of cycloolefin copolymer (a) 
A copolymerization reaction of ethylene and 
tetracyclo[4.4.0.1.sup.2,5.1.sup.7,10 ]dodecene-3 (to be sometimes 
abbreviated as "TCD-3" hereinafter) was continuously carried out with a 
one-liter polymerizer having a stirring vane. That is, the polymerizer was 
continuously fed, from its top, with a cyclohexane solution of TCD-3 at a 
rate of 0.4 lit./hour such that the concentration of TCD-3 in the 
polymerizer was 60 g/lit, a cyclohexane solution of VO(OC.sub.2 
H.sub.5)Cl.sub.2 at a rate of 0.5 lit./hour such that the concentration of 
vanadium in the polymerizer was 0.5 mmol/lit. (in this case the 
concentration of vanadium being fed was 2.86 times that of vanadium in the 
polymerizer), a cyclohexane solution of ethylaluminum sesquichloride 
[Al(C.sub.2 H.sub.5).sub.1.5 Cl.sub.1.5 ] at a rate of 0.4 lit./hour such 
that the concentration of aluminum in the polymerizer was 4.0 mmol/l, and 
cyclohexane at a rate of 0.7 lit./hour, while polymerization reaction 
liquid was continuously withdrawn from the bottom of the polymerizer such 
that the amount of polymerization liquid in the polymerizer was constantly 
1 lit. (that is, the residence time was 0.5 hour). 
Further, the reaction system was also fed with 30 lit./hour of ethylene, 10 
lit./hour of nitrogen and 0.3 lit./hour of hydrogen through a bubbling 
tube. 
The copolymerization was carried out at 10.degree. C. with circulating a 
cooling medium through a jacket externally provided to the polymerizer. 
An ethylene TCD-3 random copolymer was prepared by carrying out the 
copolymerization reaction under the above conditions. 
That is, polymerization liquid was withdrawn from the bottom of the 
polymerizer, and a cyclohexane/isopropyl alcohol mixed liquid (volume 
ratio=1/1) was added thereto to terminate the polymerization reaction. 
Then, an aqueous solution prepared by adding 5 ml of concentrated 
hydrochloric acid to 1 lit. of water and the above polymerization solution 
in a proportion of 1:1 were brought into contact by stirring them 
vigorously with a homomixer thereby to transfer a catalyst residue to a 
water phase. 
The above mixture was allowed to stand, and the water phase was removed. 
Then, the remainder was further washed with distilled water twice, and 
purified and separated. 
The resultant polymerization liquid was brought into contact, with 
vigorously stirring, with acetone of which the amount was three times that 
of the polymerization liquid, and a solid portion precipitated was 
recovered by filtration, and fully washed with acetone. Thereafter, the 
recovered solid was dried under a nitrogen current at 130.degree. C. at 
350 mmHg for 24 hours. The above procedure was continuously carried out to 
prepare an ethylene.TCD-3 random copolymer at a rate of 76 g(38 
g/lit)/hour. 
The above copolymer had an ethylene content, determined on the basis of the 
result of measurement by .sup.13 C-NMR analysis, of 70 mol %. Further, 
this copolymer was measured for an intrinsic viscosity [.eta.] in decalin 
at 135.degree. C. to show 0.61 dl/g, and it had an iodine value of 1.0 and 
TMA of 115.degree. C. 
This cycloolefin random copolymer (a) is referred to as "PO-1" hereinafter. 
PREATION EXAMPLE 2 
Polymerization example of cycloolefin copolymer (a) 
Preparation Example 1 was repeated except that the polymerizer was fed with 
ethylene at a rate of 20 lit./hour and hydrogen at a rate of 0.5 
lit./hour, to prepare an ethylene.TCD-3 copolymer. 
The above copolymer had an ethylene content, determined on the basis of the 
result of measurement by .sup.13 C-NMR analysis, of 63 mol %. Further, 
this copolymer was measured for an intrinsic viscosity [.eta.] in decalin 
at 135.degree. C. to show 0.5 dl/g, and it had an iodine value of 1.0 and 
TMA of 150.degree. C. 
This cycloolefin random copolymer (a) is referred to as "PO-2" hereinafter. 
PREATION EXAMPLE 3 
Preparation example of cycloolefin copolymer (a) 
Preparation Example 1 was repeated except that the polymerizer was fed with 
ethylene at a rate of 20 lit./hour and hydrogen at a rate of 0.3 
lit./hour, to prepare an ethylene.TCD-3 copolymer. 
The above copolymer had an ethylene content, determined on the basis of the 
result of measurement by .sup.13 C-NMR analysis, of 63 mol %. Further, 
this copolymer was measured for an intrinsic viscosity [.eta.] in decalin 
at 135.degree. C. to show 0.6 dl/g, and it had an iodine value of 1.0 and 
TMA of 150.degree. C. 
This cycloolefin random copolymer (a) is referred to as "PO-3" hereinafter. 
PREATION EXAMPLE 4 
Preparation example of cycloolefin copolymer (a) 
Preparation Example 1 was repeated except that the polymerizer was fed with 
ethylene at a rate of 10 lit./hour and hydrogen at a rate of 0.3 
lit./hour, to prepare an ethylene.TCD-3 copolymer. 
The above copolymer had an ethylene content, determined on the basis of the 
result of measurement by .sup.13 C-NMR analysis, of 56 mol %. Further, 
this copolymer was measured for an intrinsic viscosity [.eta.] in decalin 
at 135.degree. C. to show 0.8 dl/g, and it had an iodine value of 1.0 and 
TMA of 170.degree. C. 
This cycloolefin random copolymer (a) is referred to as "PO-4" hereinafter. 
PREATION EXAMPLE 5 
Preparation example of graft-modified elastomer (b) 
One part by weight of maleic anhydride and 0.2 part by weight of 
2,5-dimethyl-2,5-di(t-butylperoxy)hexyne-3 were mixed with 100 parts by 
weight of an ethylene propylene copolymer having an ethylene content of 80 
mol % and an intrinsic viscosity [.eta.], measured in decalin at 
130.degree. C., of 2.2 dl/g (this copolymer will be referred to as "MP-0" 
hereinafter), and the resultant mixture was melt-kneaded at 260.degree. C. 
with a twin-screw extruder equipped with a vent having a diameter of 30 mm 
to give a graft-modified elastomer (b). 
The above-obtained graft-modified elastomer had a maleic anhydride graft 
amount of 0.90% by weight and a tensile modulus of 80 kg/cm.sup.2. 
The above graft-modified elastomer (b) is referred to as "MP-1" 
hereinafter. 
PREATION EXAMPLE 6 
Preparation example of graft-modified elastomer (b) 
Preparation Example 5 was repeated except that the maleic anhydride was 
replaced with 1 part by weight, per 100 parts by weight of "MP-0", of 
glycidyl methacrylate and that this glycidyl methacrylate was mixed with 
0.2 part by weight of 2,5-dimethyl-2,5-di(t-butylperoxy)-hexyne-3 to give 
a graft-modified elastomer (b). 
The above-obtained graft-modified elastomer had a glycidyl methacrylate 
graft amount of 0.90% by weight and a tensile modulus of 80 kg/cm.sup.2. 
The above graft-modified elastomer (b) is referred to as "MP-2" 
hereinafter. 
PREATION EXAMPLE 7 
Preparation example of graft-modified elastomer (b) 
1 Part by weight of maleic anhydride and 0.2 part by weight of 
2,5-dimethyl-2,5-di(t-butylperoxy)hexyne-3 were mixed with 100 parts by 
weight of an ethylene propylene copolymer having an ethylene content of 80 
mol % and an intrinsic viscosity [.eta.], measured in decalin at 
130.degree. C., of 1.4 dl/g, and the resultant mixture was melt-kneaded at 
260.degree. C. with a twin-screw extruder equipped with a vent having a 
diameter of 30 mm to give a graft-modified elastomer (b). 
The above-obtained graft-modified elastomer had a maleic anhydride graft 
amount of 0.98% by weight and a tensile modulus of 80 kg/cm.sup.2. 
The above graft-modified elastomer (b) is referred to as "MP-3" 
hereinafter. 
PREATION EXAMPLE 8 
Preparation example of a compound (c) having an amino group 
Vacuum-dried .epsilon.-aminocaproic acid (to be referred to as PA-0 
hereinafter) was kept at 170.degree. C. under reduced pressure for 14 
hours to give a polymer of PA-0. This polymer had an intrinsic viscosity 
[.eta.], measured in sulfuric acid at 25.degree. C., of 0.4 dl/g. 
The above compound having an amino group is referred to as "PA-1" 
hereinafter. 
EXAMPLE 1 
10 Parts by weight of the graft-modified elastomer (MP-1) obtained in 
Preparation Example 5 and 5 parts by weight of nylon-6 (trade name: Amilan 
CM1007, supplied by Toray Industries, Inc) as a compound having an amino 
group were melt-kneaded at 250.degree. C. with a twin-screw extruder 
equipped with a vent having a diameter of 30 mm to prepare a precursor 
compound. This precursor substance and 85 parts by weight of the 
cycloolefin random copolymer (PO-1) obtained in Preparation Example 1 were 
kneaded with the above extruder at 230.degree. C. to give a polyolefin 
resin composition. 
The resultant resin composition was dried at 100.degree. C. for 8 hours, 
and then test pieces and square bars for the measurements of physical 
properties were prepared therefrom with an injection molding machine (30 
EPN, supplied by Toshiba IS) at 250.degree. C. at a mold temperature of 
70.degree. C. 
Table 1 shows the physical properties of the test pieces. 
As is clear from the results shown in Table 1, the above-obtained 
composition was excellent in impact strength, rigidity, heat resistance, 
gloss and flowability. 
COMATIVE EXAMPLE 1 
Example 1 was repeated except that 15 parts by weight of the graft-modified 
elastomer (MP-1) obtained in Preparation Example 5 and 85 parts by weight 
of the cycloolefin random copolymer (PO-1) obtained in Preparation Example 
1 were melt-kneaded with a twin-screw extruder equipped with a vent having 
a diameter of 30 mm at 230.degree. C. without using Amilan CM1007 to give 
a polyolefin resin composition. Test pieces and square bars were prepared 
from this resin composition in the same manner as in Example 1, and 
evaluated on physical properties. 
Table 1 shows the physical properties of the test pieces. 
As is clear from the results shown in Table 1, this composition showed 
excellent flowability, and the test pieces formed from this composition 
were excellent in rigidity and heat resistance. However, the impact 
strength thereof was low. 
EXAMPLE 2 
85 Parts by weight of the cycloolefin copolymer (PO-1) obtained in 
Preparation Example 1, 10 parts by weight of the graft-modified elastomer 
(MP-1) and 5 parts of a compound having an amino group (CM1007) were 
melt-kneaded with the above extruder in the same manner as in Example 1 
without preparing a precursor mixture to obtain a polyolefin resin 
composition. Test pieces and square bars were prepared from this resin 
composition in the same manner as in Example 1, and evaluated on their 
physical properties. 
Table 1 shows the physical properties of the above-obtained test pieces. 
As is clear from the results shown in Table 1, the test pieces formed from 
this composition were excellent in impact strength, rigidity, heat 
resistance and gloss, and the composition was also excellent in 
flowability. 
EXAMPLE 3 
Example 1 was repeated except that the graft-modified elastomer was changed 
to MP-2 to prepare a polyolefin resin composition. Test pieces and square 
bars were prepared from this resin composition in the same manner as in 
Example 1, and evaluated on their properties. 
Table 1 shows the physical properties of the above-obtained test pieces. 
As is clear from the results shown in Table 1, the test pieces formed from 
this composition were excellent in impact strength, rigidity, heat 
resistance and gloss, and the composition was also excellent in 
flowability. 
COMATIVE EXAMPLE 2 
Example 1 was repeated except that 15 parts by weight of the graft-modified 
elastomer (MP-2) and 85 parts by weight of the cycloolefin random 
copolymer (PO-1) were melt-kneaded with a twin-screw extruder equipped 
with a vent having a diameter of 30 mm at 230.degree. C. without using 
CM1007 to give a polyolefin resin composition. Test pieces and square bars 
were prepared from this resin composition in the same manner as in Example 
1 and evaluated on their physical properties. 
Table 1 shows the physical properties of the test pieces. 
As is clear from the results shown in Table 1, this composition showed 
excellent flowability, and the test pieces formed from this composition 
were excellent in rigidity and heat resistance. However, the impact 
strength thereof was low. 
EXAMPLE 4 
Example 1 was repeated except that the graft-modified elastomer was 
replaced with MP-3 to prepare a polyolefin resin composition. Test pieces 
and square bars were prepared from this resin composition in the same 
manner as in Example 1, and evaluated on their properties. 
Table 1 shows the physical properties of the above-obtained test pieces. 
As is clear from the results shown in Table 1, the test pieces formed from 
this composition were excellent in impact strength, rigidity, heat 
resistance and gloss, and the composition was also excellent in 
flowability. 
COMATIVE EXAMPLE 3 
15 Parts by weight of the graft-modified elastomer (MP-3) and 85 parts by 
weight of the cycloolefin random copolymer (PO-1) were melt-kneaded at 
230.degree. C. with an twin-screw extruder equipped with a vent having a 
diameter of 30 mm in the same manner as in Example 1 without using CM1007 
to obtain a polyolefin resin composition. Test pieces and square bars were 
prepared from this resin composition in the same manner as in Example 1, 
and evaluated on their physical properties. 
Table 1 shows the physical properties of the above-obtained test pieces. 
As is clear from the results shown in Table 1, the above composition was 
excellent in flowability and the test pieces formed from this composition 
were excellent in rigidity and heat resistance. However, their impact 
strength was low. 
EXAMPLE 5 
14 Parts by weight of the graft-modified elastomer (MP-1) obtained in 
Preparation Example 5 and 1 part by weight of "PA-1" as a compound having 
an amino group were melt-kneaded at 250.degree. C. with a twin screw 
extruder equipped with a vent having a diameter of 30 mm to prepare a 
precursor mixture. This precursor substance and 85 parts by weight of the 
cycloolefin random copolymer (PO-1) obtained in Preparation Example 1 were 
melt-kneaded with the above extruder to give a polyolefin resin 
composition. 
Test pieces and square bars were prepared from this resin composition in 
the same manner as in Example 1, and evaluated on their physical 
properties. 
Table 1 shows the physical properties of the above-obtained test pieces. 
As is clear from the results shown in Table 1, the test pieces formed from 
this composition were excellent in impact strength, rigidity, heat 
resistance and gloss, and the composition was also excellent in 
flowability. 
EXAMPLE 6 
12 Parts by weight of the graft-modified elastomer (MP-1) obtained in 
Preparation Example 5 and 3 parts by weight of "PA-1" obtained in 
Preparation Example 8 as a compound having an amino group were 
melt-kneaded at 250.degree. C. with a twin-screw extruder equipped with a 
vent having a diameter of 30 mm to prepare a precursor mixture. This 
precursor substance and 85 parts by weight of the cycloolefin random 
copolymer (PO-1) obtained in Preparation Example 1 were kneaded with the 
above extruder at 230.degree. C. to give a polyolefin resin composition. 
Test pieces and square bars were prepared from this resin composition in 
the same manner as in Example 1, and evaluated on their physical 
properties. 
Table 1 shows the physical properties of the above-obtained test pieces. 
As is clear from the results shown in Table 1, the test pieces formed from 
this composition were excellent in impact strength, rigidity, heat 
resistance and gloss, and the composition was also excellent in 
flowability. 
EXAMPLE 7 
10 Parts by weight of the graft-modified elastomer (MP-1) obtained in 
Preparation Example 5 and 5 parts by weight of a compound having an amino 
group, Amilan (CM1007), were melt-kneaded at 250.degree. C. with a 
twin-screw extruder equipped with a vent having a diameter of 30 mm to 
prepare a precursor mixture. This precursor substance and 85 parts by 
weight of the cycloolefin random copolymer (PO-2) obtained in Preparation 
Example 2 were kneaded with the above extruder at 230.degree. C. to give a 
polyolefin resin composition. 
Test pieces and square bars were prepared from this resin composition in 
the same manner as in Example 1, and evaluated on their physical 
properties. 
Table 1 shows the physical properties of the above-obtained test pieces. 
As is clear from the results shown in Table 1, the test pieces formed from 
this composition were excellent in impact strength, rigidity, heat 
resistance and gloss, and the composition was also excellent in 
flowability. 
COMATIVE EXAMPLE 4 
15 Parts by weight of the graft-modified elastomer (MP-1) and 85 parts by 
weight of the cycloolefin random copolymer (PO-2) were melt-kneaded at 
230.degree. C. with an twin-screw extruder equipped with a vent having a 
diameter of 30 mm in the same manner as in Example 7 without using CM1007 
to obtain a polyolefin resin composition. Test pieces and square bars were 
prepared from this resin composition in the same manner as in Example 1, 
and evaluated on their physical properties. 
Table 1 shows the physical properties of the above-obtained test pieces. 
As is clear from the results shown in Table 1, the above composition was 
excellent in flowability and the test pieces formed from this composition 
were excellent in rigidity and heat resistance. However, their impact 
strength was low. 
EXAMPLE 8 
10 Parts by weight of the graft-modified elastomer (MP-1) obtained in 
Preparation Example 5 and 10 parts by weight of a compound having an amino 
group, Amilan (CM1007), were melt-kneaded at 250.degree. C. with a 
twin-screw extruder equipped with a vent having a diameter of 30 mm to 
prepare a precursor mixture. This precursor substance and 80 parts by 
weight of the cycloolefin random copolymer (PO-2) obtained in Preparation 
Example 2 were kneaded with the above extruder at 230.degree. C. to give a 
polyolefin resin composition. 
Test pieces and square bars were prepared from this resin composition in 
the same manner as in Example 1, and evaluated on their physical 
properties. 
Table 1 shows the physical properties of the above-obtained test pieces. 
As is clear from the results shown in Table 1, the test pieces formed from 
this composition were excellent in impact strength, rigidity, heat 
resistance and gloss, and the composition was also excellent in 
flowability. 
EXAMPLE 9 
12 Parts by weight of the graft-modified elastomer (MP-1) obtained in 
Preparation Example 5 and 3 parts by weight of a compound having an amino 
group (PA-1) obtained in Preparation Example 8 were melt-kneaded at 
250.degree. C. with a twin-screw extruder equipped with a vent having a 
diameter of 30 mm to prepare a precursor mixture. This precursor substance 
and 85 parts by weight of the cycloolefin random copolymer (PO-3) obtained 
in Preparation Example 3 were kneaded with the above extruder at 
230.degree. C. to give a polyolefin resin composition. 
Test pieces and square bars were prepared from this resin composition in 
the same manner as in Example 1, and evaluated on their physical 
properties. 
Table 1 shows the physical properties of the above-obtained test pieces. 
As is clear from the results shown in Table 1, the test pieces formed from 
this composition were excellent in impact strength, rigidity, heat 
resistance and gloss, and the composition was also excellent in 
flowability. 
EXAMPLE 10 
10 Parts by weight of the graft-modified elastomer (MP-1) obtained in 
Preparation Example 5 and 5 parts by weight of a compound having an amino 
group, Amilan (CM1007), were melt-kneaded at 250.degree. C. with a 
twin-screw extruder equipped with a vent having a diameter of 30 mm to 
prepare a precursor mixture. This precursor substance and 85 parts by 
weight of the cycloolefin random copolymer (PO-3) obtained in Preparation 
Example 3 were kneaded with the above extruder at 230.degree. C. to give a 
polyolefin resin composition. 
Test pieces and square bars were prepared from this resin composition in 
the same manner as in Example 1, and evaluated on their physical 
properties. 
Table 1 shows the physical properties of the above-obtained test pieces. 
As is clear from the results shown in Table 1, the test pieces formed from 
this composition were excellent in impact strength, rigidity, heat 
resistance and gloss, and the composition was also excellent in 
flowability. 
COMATIVE EXAMPLE 5 
15 Parts by weight of the graft-modified elastomer (MP-1) and 85 parts by 
weight of the cycloolefin random copolymer (PO-3) were melt-kneaded at 
230.degree. C. with an twin-screw extruder equipped with a vent having a 
diameter of 30 mm in the same manner as in Example 10 without using CM1007 
to obtain a polyolefin resin composition. Test pieces and square bars were 
prepared from this resin composition in the same manner as in Example 1, 
and evaluated on their physical properties. 
Table 1 shows the physical properties of the above-obtained test pieces. 
As is clear from the results shown in Table 1, the above composition was 
excellent in flowability and the test pieces formed from this composition 
were excellent in rigidity and heat resistance. However, their impact 
strength was low. 
EXAMPLE 11 
10 Parts by weight of the graft-modified elastomer (MP-1) obtained in 
Preparation Example 5 and 5 parts by weight of a compound having an amino 
group, Amilan (CM1007), were melt-kneaded at 250.degree. C. with a 
twin-screw extruder equipped with a vent having a diameter of 30 mm to 
prepare a precursor mixture. This precursor substance and 85 parts by 
weight of the cycloolefin random copolymer (PO-4) obtained in Preparation 
Example 4 were kneaded with the above extruder at 230.degree. C. to give a 
polyolefin resin composition. 
Test pieces and square bars were prepared from this resin composition in 
the same manner as in Example 1, and evaluated on their physical 
properties. 
Table 1 shows the physical properties of the above-obtained test pieces. 
As is clear from the results shown in Table 1, the test pieces formed from 
this composition were excellent in impact strength, rigidity, heat 
resistance and gloss, and the composition was also excellent in 
flowability. 
COMATIVE EXAMPLE 6 
15 Parts by weight of the graft-modified elastomer (MP-1) and 85 parts by 
weight of the cycloolefin random copolymer (PO-4) were melt-kneaded at 
230.degree. C. with an twin-screw extruder equipped with a vent having a 
diameter of 30 mm in the same manner as in Example 11 without using CM1007 
to obtain a polyolefin resin composition. Test pieces and square bars were 
prepared from this resin composition in the same manner as in Example 1, 
and evaluated on their physical properties. 
Table 1 shows the physical properties of the above-obtained test pieces. 
As is clear from the results shown in Table 1, the above composition was 
excellent in flowability and the test pieces formed from this composition 
were excellent in rigidity and heat resistance. However, their impact 
strength was low. 
TABLE 1 
__________________________________________________________________________ 
Cycloolefin 
Graft Compound 
Resin 
randum modified 
having amino 
composition 
IZ FM MI Gloss 
TMA 
copolymer (a) 
elastomer (b) 
group (c) 
(a)/(b)/(c) 
(kg .multidot. cm/cm) 
(kg/cm.sup.2) 
(g/10 min.) 
(%) (.degree.C.) 
__________________________________________________________________________ 
Ex. 1 PO-1 MP-1 CM1007 85/10/5 
53 22000 
15 97 112 
Com. Ex. 1 
PO-1 MP-1 -- 85/15/0 
6 21000 
15 93 114 
Ex. 2 PO-1 MP-1 CM1007 85/10/5 
50 19000 
15 95 112 
Ex. 3 PO-1 MP-2 CM1007 85/10/5 
41 20000 
13 95 111 
Com. Ex. 2 
PO-1 MP-2 -- 85/15/0 
6 22000 
15 95 114 
Ex. 4 PO-1 MP-3 CM1007 85/10/5 
40 21000 
15 95 111 
Com. Ex. 3 
PO-1 MP-3 -- 85/15/0 
6 22500 
16 97 113 
Ex. 5 PO-1 MP-1 PA-0 85/14/1 
52 21000 
15 95 111 
Ex. 6 PO-1 MP-1 PA-1 85/12/3 
45 20500 
15 95 112 
Ex. 7 PO-2 MP-1 CM1007 85/10/5 
12 23500 
26 97 148 
Com. Ex. 4 
PO-2 MP-1 -- 85/15/0 
3 23600 
27 95 149 
Ex. 8 PO-2 MP-1 CM1007 80/10/10 
20 20000 
27 97 145 
Ex. 9 PO-3 MP-1 PA-1 85/12/3 
14 23000 
27 95 149 
Ex. 10 PO-3 MP-1 CM1007 85/10/5 
15 23400 
4 93 149 
Com. Ex. 5 
PO-3 MP-1 -- 85/15/0 
5 23000 
4 92 148 
Ex. 11 PO-4 MP-1 CM1007 85/10/5 
25 23000 
0.2 90 168 
Com. Ex. 6 
PO-4 MP-1 -- 85/15/0 
6 23300 
0.3 93 167 
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