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
2001-09-12
2004-08-10
Lipman, Bernard (Department: 1713)
Synthetic resins or natural rubbers -- part of the class 520 ser
Synthetic resins
Mixing of two or more solid polymers; mixing of solid...
C428S035500
Reexamination Certificate
active
06774190
ABSTRACT:
FIELD OF THE INVENTION
The present invention relates to ethylene copolymer compositions, more particularly to ethylene copolymer compositions which show higher heat stability and moldability as compared with conventional ethylene copolymers or ethylene copolymer compositions and from which films of high transparency, high mechanical strength and high blocking resistance can be formed.
BACKGROUND OF THE INVENTION
Ethylene copolymers have heretofore been molded by various molding methods, and used in many fields. The requirement for the characteristics of the ethylene copolymers differs depending on the molding methods and uses. For example, when an inflation film is molded at a high speed, it is necessary to select an ethylene copolymer having a high melt tension compared with its molecular weight in order to stably conduct high speed molding without fluctuation or tearing of bubbles. An ethylene copolymer is required to have similar characteristics in order to prevent sag or tearing in blow molding, or to suppress width shortage to the minimum range in T-die molding.
Further, in extrusion molding, it is important to have small stress under high shearing during extrusion in order to improve quality of molded article and reduce electric power consumption at molding.
On the other hand, Japanese Patent L-O-P Nos. 90810/1981 and 106806/1985 propose a method for improving moldability by improving the melt tension and blow ratio (die/swell ratio) of ethylene polymers obtained by using Ziegler type catalysts, especially a titanium type catalyst.
The ethylene polymers obtained by using a titanium catalyst, however, especially the low density ethylene polymers generally have problems such as their broad composition distribution and stickiness of their molded articles such as films.
Of the ethylene polymers prepared by using the Ziegler type catalysts, those obtained by using chromium type catalysts are relatively excellent in melt tension but has a defect of poor heat stability. This is thought to be caused by that the chain terminals of the ethylene polymers prepared by using the chromium type catalysts tend to become unsaturated bonds.
It is known that the ethylene polymers obtained by using a metallocene catalyst from among the Ziegler type catalysts have merits such as a narrow composition distribution and a low stickiness of their molded articles such as films. However, it is described in, for example Japanese Patent L-O-P. No. 35007/1985, that an ethylene polymer obtained by using a zirconocene compound formed from a cyclopentadienyl derivative contains one terminal unsaturated bond per molecule, and hence this ethylene polymer is presumably poor in heat stability similarly to the above-mentioned ethylene polymer obtained by using the chromium type catalyst. Further, because of its narrow composition distribution, this ethylene polymer might show poor flowability during the extrusion molding.
Accordingly, the advent of ethylene polymers having a small stress under the high-shear region, a good heat stability, a high mechanical strength and a narrow composition distribution will industrially be of great value.
The present inventors have earnestly studied in the light of the circumstances as described above. As a result, they have found that the ethylene/&agr;-olefin copolymer obtained by copolymerizing ethylene with an &agr;-olefin of 3 to 20 carbon atoms in the presence of a specific catalyst for olefin polymerization has a density, a melt flow rate (MFR), a temperature (Tm) at which its endothermic curve measured by a differential scanning calorimeter (DSC) shows the maximum peak, a flow index (FI) and an amount of a decane-soluble portion in the specific ranges, and the melt tension (MT) at 190° C. and the melt flow rate (MFR) satisfy the relation MT>2.2×MFR
−0.84
. The present inventors have also found that such an ethylene/&agr;-olefin copolymer [A-1] as mentioned above is excellent in melt tension and heat stability and has a narrow composition distribution. However, the ethylene/&agr;-olefin copolymer [A-1] is not always well-balanced between the melt tension and the flowability, so that a problem sometimes occurs when the copolymer is subjected to extrusion molding to form a film.
The present inventors have further studied and found that the following ethylene copolymer compositions (1) to (4) are excellent in heat stability, melt tension and flowability under the high-shear region, and films obtained from these compositions are excellent in transparency, mechanical strength and blocking resistance.
(1) An ethylene copolymer composition comprising the aforesaid ethylene/&agr;-olefin copolymer [A-1] and a specific low-density polyethylene [B-1] obtained by high-pressure radical polymerization.
(2) An ethylene copolymer composition comprising the aforesaid ethylene/&agr;-olefin copolymer [A-1] and a specific crystalline polyolefin [B-2].
(3) An ethylene copolymer composition comprising the aforesaid ethylene/&agr;-olefin copolymer [A-1] and a specific olefin type elastomer [B-3].
(4) An ethylene copolymer composition comprising an ethylene/&agr;-olefin copolymer composition and a specific low-density polyethylene [B-1] obtained by high-pressure radical polymerization, said ethylene/&agr;-olefin copolymer composition comprising an ethylene/&agr;-olefin copolymer [A-2] having physical properties similar to those of the aforesaid ethylene/&agr;-olefin copolymer [A-1] and an intrinsic viscosity [&eegr;] in the specific range and an ethylene/&agr;-olefin copolymer [A-3] having physical properties similar to those of the aforesaid ethylene/&agr;-olefin copolymer [A-1] and an intrinsic viscosity [&eegr;] in the specific range.
Further, the present inventors have found that an ethylene/&agr;-olefin copolymer [A-4] obtained by copolymerizing ethylene with an &agr;-olefin of 3 to 20 carbon atoms in the presence of a specific olefin polymerization catalyst which is different from the aforementioned olefin polymerization catalyst has a density, a melt flow rate (MFR), a temperature (Tm) at which its endothermic curve measured by a differential scanning calorimeter (DSC) shows the maximum peak and an amount of its decane-soluble portion in the specific ranges, and the melt tension (MT) at 190° C. and the melt flow rate (MFR) satisfy the relation MT≦2.2×MFR
−0.84
. The present inventors have also found that this ethylene/&agr;-olefin copolymer [A-4] is excellent in heat stability and has a narrow composition distribution.
As the result of further studies, the present inventors have found that the following ethylene copolymer compositions (5) to (8) are excellent in heat stability and melt tension, and films obtained from these compositions are excellent in transparency, mechanical strength and blocking resistance.
(5) An ethylene copolymer composition comprising the above-mentioned ethylene/&agr;-olefin copolymer [A-4] and a specific low-density polyethylene [B-4] obtained by high-pressure radical polymerization.
(6) An ethylene copolymer composition comprising the above-mentioned ethylene/&agr;-olefin copolymer [A-4] and a specific crystalline polyolefin [B-2].
(7) An ethylene copolymer composition comprising the above-mentioned ethylene/&agr;-olefin copolymer [A-4] and a specific olefin type elastomer [B-3].
(8) An ethylene copolymer composition comprising an ethylene/&agr;-olefin copolymer composition and a specific low-density polyethylene [B-4] obtained by high-pressure radical polymerization, said ethylene/&agr;-olefin copolymer composition comprising an ethylene/&agr;-olefin copolymer [A-5] having physical properties similar to those of the above-mentioned ethylene/&agr;-olefin copolymer [A-4] and an intrinsic viscosity [&eegr;] in the specific range and an ethylene/&agr;-olefin copolyme
Ikeyama Seiichi
Kaneshige Norio
Matsunaga Shin-ya
Takahashi Mamoru
Todo Akira
Lipman Bernard
Mitsui Chemicals Inc.
Sherman & Shalloway
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