Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Polymers from only ethylenic monomers or processes of...
Reexamination Certificate
2000-03-23
2003-09-02
Zitomer, Fred (Department: 1713)
Synthetic resins or natural rubbers -- part of the class 520 ser
Synthetic resins
Polymers from only ethylenic monomers or processes of...
C526S245000, C526S319000, C526S332000, C526S347000
Reexamination Certificate
active
06613855
ABSTRACT:
TECHNICAL FIELD
The present invention relates to a cured resin obtained by curing a polymerizable resin capable of forming thin films excellent in various characteristics, such as heat resistance, solvent resistance, low water absorption, insulating properties, low dielectric constant, and chemical resistance, in particular having a low dielectric constant, which constitutes an over coating material or interlayer insulating material for use in circuit boards to be used in various kinds of electrical machinery and apparatus, electronic parts, semiconductor devices and the like, to an insulating material comprising said cured resin, and to electrical machinery and apparatus parts and electrical machinery and apparatus in which said insulating material is used.
The range of application of said polymerizable resin and cured resin is not limited to the fields mentioned above. They can be used in various fields by making efficient use of their excellent heat resistance, solvent resistance and other characteristics, in particular in fields which require thin films other than the fields mentioned above.
BACKGROUND ART
Various insulating materials, for example passivation films, solder resists, resists for plating, interlayer insulating materials and moisture-proof protective films, are known as over coating materials, interlayer insulating materials or the like for use in semiconductors, ICs, hybrid ICs, wiring substrates, display devices, display parts and the like in the electronics industry. The recent trends toward miniaturization, high density constitution and high speed operation of electronic parts require that such insulating materials should have higher performance characteristics and higher reliability.
Epoxy resin compositions, polyimide resins and polybutadiene compositions, among others, are known as the resin compositions constituting such insulating materials. However, epoxy resin compositions and polyimide resins have a problem in moisture resistance and a problem concerning their electric characteristics, in particular their high dielectric characteristics in high frequency ranges. Polybutadiene resins have good moisture resistance and dielectric characteristics but have a problem in heat resistance.
Novel materials are thus demanded to meet such characteristics required for over coating materials, interlayer insulating materials and like insulating materials. Attempts have been made to use polyolefin resins and polyphenylene ether resins, which have good electrical characteristics. However, polyolefin resins and polyphenylene ether resins are thermoplastic resins and therefore their heat resistance is not fully satisfactory. Another problem is that, in multilayer formation, the lower layer is damaged by the solvent.
To solve such problems, a method of improving the heat resistance, solvent resistance and other properties of copolymers of a norbornene type monomer and ethylene by sulfur crosslinking, organic peroxide crosslinking, electron beam crosslinking or radiation crosslinking, for instance, has been proposed (Japanese Kokai Publication Sho-62-34924). However, it was revealed that such a method encounters problems in applying it to over coating materials, interlayer insulating materials or like insulating materials in view of residual sulfur, storage stability of a mixture and necessity of a considerable equipment investment, among others.
A method of improving the heat resistance, solvent resistance and other properties by introducing an epoxy group to cyclic olefin resins, typically norbornene resins, and curing the resulting resin compositions, with a crosslinking agent dispersed therein, has also been proposed (Japanese Kokai Publication Hei-8-259784). However, said method has a problem concerning dielectric characteristics because the cured resins obtained by such a method using an epoxy group and a crosslinking agent, which are highly polalizable, as crosslinking functional groups.
Further, propargyl- or allyl-substituted polyphenylene ethers, double bond- or double bond-containing polyphenylene ethers and unsaturated carboxylic acid- or acid anhydride-modified polyphenylene ethers have been proposed (Japanese Kokai Publication Hei-1-69628, Japanese Kokai Publication Hei-1-69629, Japanese Kokai Publication Hei-1-113425, Japanese Kokai Publication Hei-1-113426, Japanese Kokai Publication Hei-1-239017, etc.). These, however, are poor in curing reactivity, in particular curing reactivity in oxygen (air), since an allyl group, olefinically unsaturated bond or unsaturated carboxylic acid is used as their curing functional group. For attaining satisfactory curing, there is a limitation that it is necessary to conduct curing in an inert gas atmosphere such as nitrogen.
SUMMARY OF THE INVENTION
In view of the foregoing, the present invention has for its object to provide a polymerizable resin capable of forming a cured resin suited for use as an over coating material, interlayer insulating material or the like and excellent in various characteristics, such as heat resistance, solvent resistance, low water absorption, insulating properties, low dielectric constant, adhesion, chemical resistance and processability, a cured resin obtained by said polymerizable resin, an insulator comprising said cured resin, and electrical machinery and apparatus parts and electrical machinery and apparatus in which said insulator is used.
The first aspect of the present invention is concerned with a polymerizable resin which comprises a copolymer of a monomer (1) represented by the general formula (1) given below and one or more monomers selected from the group consisting of monomers (2) to (6) respectively represented by the general formulas (2) to (6) given below, wherein the weight ratio of the monomer (1)/[sum total of monomers (2) to (6)] is 5/95 to 95/5 and the number average molecular weight of said copolymer is 2000 to 1000000;
[In the formula, R
1
represents a hydrogen atom or a methyl group, X represents COOR
2
or OR
2
, R
2
represents an alkylene group containing 1 to 6 carbon atoms and may optionally be substituted with a hydrokyl group or a halogen atom, and Z represents an alkenyl group containing 2 to 5 carbon atoms.];
[In the formula, n is an integer of 1 to 10. ];
[In the formula, R
1
represents a hydrogen atom or a methyl group, m is an integer of 0 to 6 and n is an integer of 1 to 10. ];
[In the formula, R
1
represents a hydrogen or fluorine atom, R
4
represents a hydrogen, chlorine or fluorine atom and R
5
represents a hydrogen or fluorine atom or a trifluoromethyl group.];
[In the formula, R
1
represents a hydrogen atom or a methyl group, T represents COOR
6
or (R
6
1
and R
6
represents a cyclic alkyl or cyclic alkenyl group containing 3 to 15 carbon atoms and may partly be substituted with a hydroxyl group or a halogen atom.];
[In the formula, R
1
represents a hydrogen atom or a methyl group, W represents an alkyl group, a hydroxyl group or a halogen atom and k is an integer of 0 to 5.];
The second aspect of the present invention is concerned with a method of producing a polymerizable resin which comprises copolymerizing the monomer (1) represented by the above general formula (1) and one or more monomers selected from the monomers (2) to (6) respectively represented by the above general formulas (2) to (6) in a proportion such that the weight ratio of the monomer (1)/[sum total of monomers (2) to (6) ] amounts to 5/95 to 95/5.
The third aspect of the present invention is concerned with a polymerizable resin which comprises one resin or a mixture of two or more resins selected from the group consisting of a cyclic olefin resin (A
0
), a resin (A
1
) prepared by substitution of at least one hydrogen atom of a methyl, methylene or methine group in said cyclic olefin resin (A
0
) with an organic group represented-by the general formula (7) given below and having a number average molecular weight of 2000 to 1000000, a polyphenylene ether resin (B
0
), a resin (B
1
) pr
Inoue Masahito
Saito Takao
Satake Munekazu
Sanyo Chemical Industries Ltd.
Zitomer Fred
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