Polyphenylene ether resin composition

Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Processes of preparing a desired or intentional composition...

Reexamination Certificate

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C524S145000

Reexamination Certificate

active

06469077

ABSTRACT:

FIELD OF THE INVENTION
The present invention relates to a polyphenylene ether resin composition. More specifically, the present invention relates to a polyphenylene ether resin composition having superior heat resistance and flame resistance, and wherein the flame resistance is remarkable when the resin composition is formed into a thin molded product.
BACKGROUND OF THE INVENTION
Polyphenylene ether resins are superior in their mechanical properties, electric properties, heat resistance, hydrolysis resistance and dimensional stability, and are extensively used as thermoplastic engineering plastic resins.
As a technique of imparting flame resistance to polyphenylene ether resins, there is known a composition comprising a polyphenylene ether resin and a phosphate flame retardant. For example, Japanese Patent Application Kokai (JP-A) No. 57-207641 discloses a flame resisting polyphenylene ether resin composition comprising a polyphenylene ether resin, a triphenyl phosphate and a polyphosphate, and teaches therein that a total amount of both the phosphates is preferably from 3 to 15% by weight based on the total amount of the polyphenylene ether resin and both the phosphates. Further, EP0767204-A discloses a flame resisting polyphenylene ether resin composition comprising a polyphenylene ether resin, a bisphenol A type condensed phosphate and a monophosphate.
Each of the references referred to above is incorporated herein by reference in its entirety.
However, the composition disclosed in JP-A 57-207641 possesses a problem in that when the composition is formed into a thin molded product such as an insulating sheet suitably used for electric and electronic parts, its flame resistance is not sufficient. Similarly, the composition disclosed in EP 0767204-A possesses a problem that makes it necessary to use a large amount of the bisphenol A type condensed phosphate in order to obtain a satisfactory flame resistance (because the content of phosphorus in the bisphenol A type condensed phosphate is low). As such, the heat resistance of the resin composition obtained is made insufficient, and therefore, it is difficult to obtain a resin composition that is well-balanced both in flame resistance and heat resistance.
SUMMARY OF THE INVENTION
Accordingly, an object of the present invention is to provide a polyphenylene ether resin composition that is superior both in its heat resistance and its flame resistance, particularly in the flame resistance of a thin molded product obtained therefrom. In thepresent invention, the term “thin molded product” is understood to mean a molded product having a thickness of usually not more than about 1 mm.
The present inventors have undertaken extensive studies with respect to studying the heat resistance and flame resistance of polyphenylene ether resin compositions. As a result, it has been found that a resin composition comprising a polyphenylene ether resin and two specific kinds of phosphorus-containing compounds can answer the object mentioned above, and thereby the present invention has been obtained.
The present invention provides a polyphenylene ether resin composition, comprising:
a component (A) containing a polyphenylene ether resin;
a component (B) containing a phosphate compound represented by the following,formula (I); and
a component (C) containing a condensed phosphate compound represented by the following formula (II),
wherein R
1
, R
2
and R
3
are independently of one another an alkyl group having 1 to 20 carbon atoms, a cycloalkyl group having 3 to 20 carbon atoms, an aryl group having 6 to 20 carbon atoms, an alkoxy group having 1 to 20 carbon atoms or a hydroxyl group; R
4
, R
5
, R
6
and R
7
are independently of one another a hydrogen atom, an alkyl group having 1 to 20 carbon atoms, a cycloalkyl group having 6 to 20 carbon atoms, an aryl group having 6 to 20 carbon atoms, an alkoxy group having 1 to 20 carbon atoms or a hydroxyl group, provided that a case of R
4
=R
5
=R
6
=R
7
=H is excluded; n is an integer of not less than 1; Z is an organic group having 1 to 10 carbon atoms; and q is an integer of from 0 to 4; and wherein said composition contains a content of phosphorus therein of from about 1.8 to 5% by weight based on the total weight of the polyphenylene ether resin composition.
The present invention further provides a thin molded product obtained from the polyphenylene ether resin composition as mentioned above and provides an insulating sheet of the thin molded product.
Further scope of applicability of the present invention will become apparent from the detailed description given hereinafter. However, it should be understood that the detailed description and specific examples, while indicating preferred embodiments of the invention, are given by way of illustration only, since various changes and modifications within the spirit and scope of the invention will become apparent to those skilled in the art from this detailed description.
DETAILED DESCRIPTION OF THE INVENTION
The component (A), that is, the polyphenylene ether resin used in the present invention, is a homopolymer resin or a copolymer resin obtained by oxidatively polymerizing at least one phenol compound represented by the following formula (III) with oxygen or an oxygen-containing gas with the aid of an oxydative coupling catalyst,
wherein R
8
, R
9
, R
10
, R
11
and R
12
are independently of one another a hydrogen atom, a halogen atom, a hydrocarbon group or substituted hydrocarbon group, provided that at least one of them is always a hydrogen atom.
Examples of R
8
, R
9
, R
10
, R
11
and R
12
in the formula (III) are hydrogen, chlorine, bromine, fluorine, iodine, methyl, ethyl, n- or iso-propyl, pri-, sec- or t-butyl, hydroxyethyl, phenylethyl, benzyl, hydroxymethyl, carboxyethyl, methoxycarbonylethyl, cyanoethyl, phenyl, methylphenyl, dimethylphenyl, ethylphenyl and allyl.
Examples of the phenol compound represented by the formula (III) are phenol, o-, m- or p-cresol, 2,6-, 2,5-, 2,4- or 3,5-dimethylphenol, 2-methyl-6-phenylphenol, 2,6-diphenylphenol, 2,6-diethylphenol, 2-methyl-6-ethylphenol, 2,3,5-, 2,3,6- or 2,4,6-trimethylphenol, 3-methyl-6-t-butylphenol, thymol and 2-methyl-6-allylphenol. Among these phenol compounds, 2,6-dimethylphenol, 2,6-diphenylphenol, 3-methyl-6-t-butylphenol and 2,3,6-trimethylphenol are preferred.
The phenol compound represented by the formula (III) may be copolymerized with a polyhydric aromatic compound such as bisphenol-A, resorcinol, hydroquinone and novolak resins to prepare a copolymer. In the present invention, the copolymer may be also used as the polyphenylene ether resin according to the present invention.
The oxidative coupling catalyst used for the oxidative (co)polymerization of said phenol compound is not particularly limited, and any catalyst having a polymerizing ability can be used.
As a process for oxidatively (co)polymerizing the phenol compound to produce the polyphenylene ether resin, there are exemplified those disclosed in, for example, U.S. Pat. Nos. 3,306,874, 3,306,875 and 3,257,357, Japanese Patent Publication (JP-B) No. 52-17880, Japanese Patent Application Kokai (JP-A) Nos. 50-51197 and 1-304119. Each of the references referred to above is incorporated herein by reference in its entirety.
Specific examples of the polyphenylene ether resin used in the present invention are poly(2,6-dimethyl-1,4-phenylene ether), poly(2,6-diethyl-1,4-phenylene ether), poly(2-methyl-6-ethyl-1,4-phenylene ether), poly(2-methyl-6-propyl-1,4-phenylene ether), poly(2,6-dipropyl-1,4-phenylene ether), poly(2-ethyl-6-propyl-1,4-phenylene ether), poly(2,6-dibutyl-1,4-phenylene ether), poly(2,6-dipropenyl-1,4-phenylene ether), poly(2,6-dilauryl-1,4-phenylene ether), poly(2,6-diphenyl-1,4-phenylene ether), poly(2,6-dimethoxy-1,4-phenylene ether), poly(2,6-diethoxy-1,4-phenylene ether), poly(2-methoxy-6-ethoxy-1,4-phenylene ether), poly(2-ethyl-6-stearyloxy-1,4-phenylene ether), poly(2-methyl-6-phenyl-1,4-phenylene ether), poly(2-methyl-1,4-phenylene ether), poly(2-ethoxy-1,4-phenylene ethe

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