Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Mixing of two or more solid polymers; mixing of solid...
Reexamination Certificate
2001-06-20
2004-02-24
Seidleck, James J. (Department: 1711)
Synthetic resins or natural rubbers -- part of the class 520 ser
Synthetic resins
Mixing of two or more solid polymers; mixing of solid...
C525S211000, C525S216000, C525S097000, C524S553000, C524S554000, C526S160000, C526S170000, C526S347000
Reexamination Certificate
active
06696527
ABSTRACT:
TECHNICAL FIELD
The present invention relates to an olefin copolymer and to films and sheets formed of the olefin copolymer. Precisely, it relates to an olefin ter-copolymer which comprises a cyclic olefin, an aromatic vinyl compound and an aliphatic &agr;-olefin having from 2 to 20 carbon atoms in a specific compositional ratio and which has a glass-transition temperature (Tg) of lower than 60° C., and to films and sheets formed of the copolymer.
BACKGROUND ART
Soft polyvinyl chloride is desired to be substituted with chlorine-free olefin resins, in view of its environmental problems of wastes, etc. For olefin resins, for example, proposed are copolymers of propylene and &agr;-olefins.
On the other hand, few ter-copolymers comprising a cyclic olefin, an aromatic vinyl compound and an &agr;-olefin have heretofore been known. A ter-copolymer of that type is disclosed in Japanese Patent Laid-Open No. 287713/1998. However, it is a hard resin for optical materials and could not be a substitute for soft polyvinyl chloride.
The invention is to provide a novel olefin copolymer which has a suitable modulus of elasticity and can be a substitute for soft polyvinyl chloride as a soft resin and which has good elastic recovery and transparency, and also to provide films and sheets formed of the copolymer.
DISCLOSURE OF THE INVENTION
We, the present inventors have assiduously studied, and, as a result, have found out an olefin copolymer that solves the above-mentioned problems and also films and sheets formed of the copolymer, and have completed the present invention. The copolymer is a novel olefin ter-copolymer that comprises a cyclic olefin, an aromatic vinyl compound and an aliphatic &agr;-olefin having from 2 to 20 carbon atoms in a specific compositional ratio and has a glass transition temperature (Tg) of lower than 60° C. Specifically, the invention provides an olefin copolymer mentioned below and films and sheets formed of the copolymer.
1. An olefin copolymer comprising [A] a cyclic olefin, [B] an aromatic vinyl compound and [C] an aliphatic &agr;-olefin having from 2 to 20 carbon atoms, which is characterized in that (1) the component [A] accounts for from 0.1 to 30 mol %, the component [B] accounts for from 0.1 to 49.9 mol %, and the total of the components [A] and [B] accounts for from 0.2 to 50 mol %, and (2) the copolymer has a glass transition temperature Tg of lower than 60° C.
2. The olefin copolymer of above 1, wherein the component [A] accounts for from 0.1 to 10 mol %, the component [B] accounts for from 0.1 to 45 mol %, and the total of the components [A] and [B] accounts for from 0.2 to 50 mol %.
3. The olefin copolymer of above 1 or 2, of which the glass transition temperature Tg is lower than 30° C.
4. The olefin copolymer of any of above 1 to 3, of which the limiting viscosity [&eegr;] measured in decalin at 135° C. falls between 0.01 and 20 dl/g.
5. The olefin copolymer of any of above 1 to 4, of which the tensile modulus is at most 600 MPa.
6. The olefin copolymer of any of above 1 to 5, of which the internal haze is at most 20%.
7. The olefin copolymer of any of above 1 to 6, which is obtained by polymerizing a cyclic olefin, an aromatic vinyl compound and an aliphatic &agr;-olefin having from 2 to 20 carbon atoms in the presence of an olefin polymerization catalyst that comprises (D) at least one selected from transition metal compounds of Groups 4 to 6 of the Periodic Table and transition metal compounds of Groups 8 to 10 of the Periodic Table of the following general formulae (1) to (4), and (E) at least one selected from a compound group of (e-1) oxygen-containing organometallic compounds, (e-2) ionic compounds capable of reacting with the transition metal compounds to form ionic complexes, and (e-3) clay, clay minerals and ion-exchanging layered compounds:
Q
1
a
(C
5
H
5−a−b
R
1
b
)(C
5
H
5−a−c
R
2
c
)M
1
X
1
Y
1
(1)
Q
2
a
(C
5
H
5−a−d
R
3
d
)Z
1
M
1
X
1
Y
1
(2)
(C
5
H
5−e
R
4
e
)M
1
X
1
Y
1
W
1
(3)
L
1
L
2
M
2
X
1
Y
1
(4)
wherein Q
1
represents a bonding group that crosslinks the two conjugated five-membered cyclic ligands (C
5
H
5−a−b
R
1
b
) and (C
5
H
5−a−c
R
2
c
); Q
2
represents a bonding group that crosslinks the conjugated five-membered cyclic ligand (C
5
H
5−a−d
R
3
d
) and the group Z
1
; R
1
, R
2
, R
3
and R
4
each represents a hydrocarbon group, a halogen atom, an alkoxy group, a silicon-containing hydrocarbon group, a phosphorus-containing hydrocarbon group, a nitrogen-containing hydrocarbon group, or a boron-containing hydrocarbon group; and a plurality of these groups, if any, may be the same or different, and may be bonded to each other to form a cyclic structure; a represents 0, 1 or 2; b, c and d each represents an integer of from 0 to 5 when a=0, or an integer of from 0 to 4 when a=1, or an integer of from 0 to 3 when a=2; e is an integer of from 0 to 5; M
1
represents a transition metal of Groups 4 to 6 or Groups 8 to 10 of the Periodic Table; M
2
represents a transition metal of Groups 8 to 10 of the Periodic Table; L
1
and L
2
each represents a covalent-bonding or coordination-bonding ligand, and they may be bonded to each other; X
1
, Y
1
, Z
1
and W
1
each represents a covalent-bonding or ionic-bonding ligand, and X
1
, Y
1
and W
1
may be bonded to each other.
8. Films and sheets formed of the olefin copolymer of any of above 1 to 7.
BEST MODES OF CARRYING OUT THE INVENTION
The invention is the olefin copolymer mentioned above, including films and sheets formed of the copolymer. The invention is described in detail hereinunder.
1. Olefin Copolymer
The olefin copolymer of the invention comprises [A] a cyclic olefin, [B] an aromatic vinyl compound and [C] an aliphatic &agr;-olefin having from 2 to 20 carbon atoms, and is characterized in that;
(1) the component [A] accounts for from 0.1 to 30 mol %, the component [B] accounts for from 0.1 to 49.9 mol %, and the total of the components [A] and [B] accounts for from 0.2 to 50 mol %, and (2) the copolymer has a glass transition temperature Tg of lower than 60° C.
The olefin copolymer of the invention is a random ter-copolymer comprising the above-mentioned components [A], [B] and [C]. Its composition generally satisfies the above-mentioned (1), but is preferably such that the component [A] accounts for from 0.1 to 10 mol %, the component [B] accounts for from 0.1 to 45 mol %, and the total of the components [A] and [B] accounts for from 0.2 to 50 mol %.
If the amount of the component [A] therein is smaller than 0.1 mol %, the transparency of the copolymer is poor. If, however, it is larger than 30 mol %, the glass transition temperature of the copolymer is high and the copolymer could not serve as a soft resin. If the amount of the component [B] therein is larger than 49.9 mol %, the glass transition temperature of the copolymer is high and the copolymer could not serve as a soft resin. If the total of the components [A] and [B] is smaller than 0.2 mol %, the copolymer will inevitably have a melting point of the crystal caused by the component [C] therein, and could not serve as a soft resin. On the other hand, if the total of the components [A] and [B] is larger than 50 mol %, the glass transition temperature of the copolymer is high and the copolymer could not serve as a soft resin. Regarding the composition of the ter-copolymer, it is desirable that the amount of the component [A] is larger than that of the component [B] for better transparency of the copolymer.
The olefin copolymer of the invention has a glass transition point (Tg) of lower than 60° C., but preferably lower than
Ishihara Nobuhide
Matsumoto Jun-ichi
Tani Noriyuki
Yokota Kiyohiko
Asinovsky Olga
Idemitsu Petrochemical Co. Ltd.
Seidleck James J.
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