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
2000-09-20
2002-10-01
Niland, Patrick D. (Department: 1714)
Synthetic resins or natural rubbers -- part of the class 520 ser
Synthetic resins
Mixing of two or more solid polymers; mixing of solid...
C428S441000, C428S461000, C428S500000, C525S071000, C525S074000, C525S088000, C525S240000
Reexamination Certificate
active
06458890
ABSTRACT:
BACKGROUND OF THE INVENTION
The present invention relates to 4-methyl-1-pentene polymer compositions. It also relates to the 4-methyl-1-pentene polymer compositions showing excellent adhesion to a 4-methyl-1-pentene polymer layer and a polar-group-containing resin layer and laminates using such compositions.
Up to the present, 4-methyl-1-pentene polymer is used in mold-releasing film, printed circuit mold-releasing materials, various containers, etc. because of its heat resistance, chemical resistance, mold-releasing properties, transparency and other properties. However, in those application areas which require mechanical strength, gas barrier properties and high-temperature mechanical strength, among other properties, it has been hoped that improvement will be made in 4-methyl-1-pentene polymer.
One example of the attempt to give such properties to 4-methyl-1-pentene polymer is to laminate 4-methyl-1-pentene polymer and a polar-group-containing resin such as ethylene/vinyl alcohol copolymer and polyamide. Ethylene/vinyl alcohol copolymer and polyamide, among others, have excellent gas barrier properties, and it is expected that the lamination of 4-methyl-1-pentene polymer and a polar-group-containing resin such as ethylene/vinyl alcohol copolymer and polyamide will make an improvement in the gas barrier properties possible. Furthermore, polyamide, particularly biaxially-oriented polyamide, shows excellent rigidity, toughness, impact resistance and other properties, and it is expected that these properties of 4-methyl-1-pentene polymer laminates will be improved by laminating such polyamide.
However, a two-layer lamination of a 4-methyl-1-pentene polymer layer and a polar-group-containing resin layer is not fit for practical use because the bonding of the two materials is not accomplished.
Attempts to bond these two materials have been made in the past. For example, Japanese Laid-open Patent Publication HEI 2-107438 discloses as an example a resin composition comprising an ethylene/&agr;-olefin random copolymer, a tackifier and a modified polyolefin as an intermediate layer of these laminates.
Moreover, the Japanese Laid-open Patent Publication HEI 2-107438 discloses that polybutene-1 and/or 4-methyl-1-pentene polymer is blended with a modified polyolefin at least in one layer in order that the polyolefin layer and the nylon layer are bonded with each other.
However, such conventional technology was not entirely satisfactory in that the level of the adhesion achieved by it was low and the heat resistance of the structure bonded by it was also low.
SUMMARY OF THE INVENTION
For the sake of resolving the problem as described above, the object of the present invention is to provide adhesive compositions which firmly bonds with the polar-group-containing resin layer and has excellent heat resistance, particularly adhesive compositions showing excellent adhesion to both of the 4-methyl-1-pentene polymer layer and the polar-group-containing resin layer, and those laminates using them which have excellent interlaminar adhesion.
Other and further objects, features and advantages of the present invention will appear more fully from the following description.
According to the present invention, the 4-methyl-1-pentene polymer composition comprises 25 to 95 wt % of a 4-methyl-1-pentene polymer (A) and 5 to 75 wt % of a modified polyolefin resin (B) comprising a mixture of an unsaturated carboxylic acid-modified &agr;-olefin polymer (B-1) whose &agr;-olefin is selected from a group of propylene, butene-1 and 4-methyl-1-pentene and an unsaturated carboxylic acid-modified ethylene/&agr;-olefin copolymer (B-2).
Furthermore, the 4-methyl-1-pentene polymer composition of the present invention comprises 25 to 90 wt % of a 4-methyl-1-pentene polymer (A); 0.1 to 20 wt % of an unsaturated carboxylic acid-modified &agr;-olefin polymer (B-1) whose &agr;-olefin is selected from the group of propylene, butene-1 and 4-methyl-1-pentene; 4 to 60 wt % of an unsaturated carboxylic acid-modified ethylene/&agr;-olefin copolymer (B-2); and 5 to 50 wt % of a butene-1 polymer (C).
Moreover, the 4-methyl-1-pentene polymer composition of the present invention comprises 26 to 96 wt % of a 4-methyl-1-pentene polymer (A′) at least part of which is modified with unsaturated carboxylic acid, whose rate of modification (in the weight ratio of the unsaturated carboxylic acid in the polymer to the polymer) may be 0.1 to 5 wt % and whose melt flow rate may be 5 to 500 g/min as determined under the conditions of a temperature being 260° C. and a load being 5 kg in accordance with ASTM D1238; and 4 to 74 wt % of an unsaturated carboxylic acid-modified ethylene/&agr;-olefin copolymer (B-2).
In addition, the 4-methyl-1-pentene polymer composition of the present invention comprises 26 to 91 wt % of a 4-methyl-1-pentene polymer (A′) at least part of which is modified with unsaturated carboxylic acid, whose rate of modification may be 0.1 to 5 wt % and whose melt flow rate may be 5 to 500 g/min as determined under the conditions of a temperature being 260° C. and a load being 5 kg in accordance with ASTM D1238; 4 to 60 wt % of an unsaturated carboxylic acid-modified ethylene/&agr;-olefin copolymer (B-2); and 5 to 50 wt % of a butene-1 polymer (C).
The present invention provides laminates comprising onto a polar-group-containing resin layer and the aforementioned 4-methyl-1-pentene polymer composition layer laminated thereto.
Furthermore, the present invention provides laminates comprising a 4-methyl-1-pentene polymer layer, a polar-group-containing resin layer, and a layer of the aforementioned 4-methyl-1-pentene polymer composition as the intermediate layer.
According to the present invention, adhesives using the aforementioned 4-methyl-1-pentene polymer composition are provided.
DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS
The 4-methyl-1-pentene polymer composition of the present invention uses a 4-methyl-1-pentene polymer (A) and (B), as a modified polyolefin resin, a mixture of an unsaturated carboxylic acid-modified &agr;-olefin polymer whose &agr;-olefin is selected from a group of propylene, butene-1 and 4-methyl-1-pentene and an unsaturated carboxylic acid-modified ethylene/&agr;-olefin copolymer.
Given below is a detailed description of the components of the 4-methyl-1-pentene polymer composition of the present invention.
(A) 4-Methyl-1-Pentene Polymer
The 4-methyl-1-pentene polymer used in the present invention is a homopolymer of 4-methyl-1-pentene or a copolymer of 4-methyl-1-pentene and another &agr;-olefin , such as the &agr;-olefins having 2 to 20 carbon atoms such as ethylene, propylene, 1-butene, 1-hexene, 1-octene, 1-decene, 1-tetradecene and 1-octadecene, for example. The 4-methyl-1-pentene/&agr;-olefin copolymer used in the present invention is normally a copolymer made up primarily of 4-methyl-1-pentene containing not less than 85 mol%, preferably not less than 90 mol% of the 4-methyl-1-pentene component. When the amount of the 4-methyl-1-pentene component is within this range, the resultant composition shows excellent heat resistance and adhesion.
The melt flow rate (MFR) of the 4-methyl-1-pentene polymer (A) used in the present invention is preferably in a range of 1 to 400 g/10 min, more preferably 10 to 300 g/10 min, as determined under the conditions of a temperature being 260° C. and a load being 5 kg in accordance with ASTM D1238.
(B) Modified Polyolefin Resin
The modified polyolefin resin of the present invention comprises a mixture of an unsaturated carboxylic acid-modified &agr;-olefin polymer (B-1) whose &agr;-olefin is selected from a group of propylene, butene-1 and 4-methyl-1-pentene and an unsaturated carboxylic acid-modified ethylene/&agr;-olefin copolymer (B-2):
(B-1) Unsaturated Carboxylic Acid-modified &agr;-Olefin Polymer
The unsaturated carboxylic acid-modified &agr;-olefin polymer used in the present invention comprises a one whose &agr;-olefin is selected from a group of propylene, butene-1 and 4-methyl-1-pentene. Specifically, the &agr;-olefin polymer, the base polyme
Noritomi Katsumi
Takata Toshimasa
Birch & Stewart Kolasch & Birch, LLP
Mitsui Chemicals Inc.
Niland Patrick D.
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