JPH046221B2 - - Google Patents

Description

[Detailed description of the invention]

The present invention relates to a flame-retardant polyphenylene ether composition that has excellent heat resistance, oil resistance, and moldability. Polyphenylene ether is a resin that has attracted much attention in recent years because of its excellent mechanical properties, electrical properties, and heat resistance, as well as its low water absorption and good dimensional stability. However, since polyphenylene ether resin alone generally has poor processability and impact strength, in many industrial applications it is used as a blend with polystyrene or rubber-reinforced polystyrene. Furthermore, it is known that compositions made by blending polystyrene into these polyphenylene ether resins have poor oil resistance. A polyphenylene ether composition with good oil resistance was published in Japanese Patent Application Laid-open No. 1983-
No. 36150. However, as mentioned above, it is also known that compositions obtained by blending other components with polyphenylene ether resin do not lose their self-extinguishing properties and require addition of flame retardant properties. For example, for a composition of polyphenylene ether resin and polystyrene,
Special Publication Publication No. 49 (1973), which has the following proposals regarding flame retardants:
-5220, Japanese Patent Publication No. 53-418 and Japanese Patent Publication No. 53-
No. 73248 proposes the use of aromatic phosphoric acid ester as a flame retardant, JP-A-48-39014 proposes the use of aromatic halides and antimony trioxide, and JP-B No. 48-38768 proposes the use of aromatic phosphoric acid esters as flame retardants. There is a proposal to use a group phosphoric acid ester in combination with an aromatic halide and antimony trioxide. However, as mentioned above, the compositions obtained by carrying out these suggestions all have the drawback of poor oil resistance. In addition, the addition of aromatic phosphate esters has the disadvantage of lowering heat resistance. In addition, the aromatic halides that have been proposed in the past generally have poor thermal stability and are undesirable in practical terms, such as when they are thermally decomposed, metal-corrosive acid gas is generated, and at the same time, the added aromatic halides themselves bleed out onto the resin surface. It has its drawbacks.
Furthermore, JP-A No. 57-165448 proposes adding red phosphorus to a composition containing polyphenylene ether resin, polyamide, and styrene-maleic anhydride copolymer, but this method does not have sufficiently good hot water resistance. It's hard to say. The present inventors have arrived at the present invention as a result of extensive studies aimed at improving the drawbacks of the above-mentioned flame retardant compositions and obtaining a flame retardant composition with good oil resistance that is mainly composed of polyphenylene ether resin. . That is, the present invention is a copolymer of (a) polyphenylene ether resin, (b) polystyrene, (c) polyamide, and (d) anhydride and/or imidized product of styrene and α,β-unsaturated dicarboxylic acid. By blending (e) halogenated polystyrene and (f) antimony-containing compound into the resin composition, it has good oil resistance, heat resistance, hot water resistance, metal corrosion resistance, and bleed-out resistance. The invention was completed by the discovery that a flame retardant composition of the following could be obtained. More specifically, the present invention comprises (a) 20 to 70 parts by weight of polyphenylene ether resin, (b) 0 to 70 parts by weight of polystyrene.
60 parts by weight, (c) 5 to 70 parts by weight of polyamide, (d) Copolymer of styrene and anhydride of α,β-unsaturated dicarboxylic acid and/or imidide of α,β-unsaturated dicarboxylic acid 3 -40 parts by weight of the resin composition, (e) a halogenated polymer having a structure obtained by polymerizing a monomer represented by the following general formula.

[Formula] (where R is hydrogen, halogen, lower alkyl, or halogenated lower alkyl, and X ₁ to _{X 5} are vinyl,
halogen, hydrogen, lower alkyl halogenated lower alkyl, and at least one of X ₁ to _{X 5} is a halogen) 3 to 40 parts by weight of listyrene and (f) 0 to 20 parts by weight of an antimony-containing compound are added. The present invention provides a composition comprising: The polyphenylene ether resin referred to in the present invention has the general formula [] or [].

【formula】

[Formula] (R ₁ , R ₂ , R ₃ , R ₄ , R ₅ and R ₆ are the same or different
Alkyl having 1 to 4 carbon atoms excluding tert-butyl group,
(Aryl group, halogen atom, hydrogen atom, etc., and R ₅ and R ₆ are not hydrogen atoms at the same time) represents a homopolymer or copolymer having a repeating unit represented by It can be obtained by reacting raw material phenol with oxygen in the presence of a manganese complex. Specific examples of polyphenylene ether resins that can be used in the present invention include poly(2,6-dimethyl-
1,4-phenylene)ether, poly(2,6-
Diethyl-1,4-phenylene ether, poly(2,6-dichloro-1,4-phenylene) ether, poly(2,6-dibromo-1,4-phenylene) ether, poly(2-methyl-6) -ethyl-1,4-phenylene) ether, poly(2-chloro-6-methyl-1,4-phenylene) ether, poly(2-methyl-6-isopropyl-1,
4-phenylene)ether, poly(2,6-di-
n-propyl-1,4-phenylene) ether,
Poly(2-chloro-6-bromo-1,4-phenylene) ether, poly(2-chloro-6-ethyl-1,4-phenylene) ether, poly(2-chloro-6-ethyl-1,4- phenylene) ether, poly(2-methyl-1,4-phenylene) ether, poly(2-phenyl-1,4-phenylene) ether, poly(2-methyl-6-phenyl-1,4-phenylene) ether, A polyphenylene ether resin obtained by copolymerizing an alkyl-substituted phenol such as poly(2-bromo-6-phenyl-1,4-phenylene)ether and 2,3-6-trimethylphenol with, for example, 0-cresol. Examples include polyphenylene ether copolymer as a main component. Furthermore, these may be grafted with a monomer mainly composed of styrene. The polyphenylene ether resin is used in an amount of 20 to 70 parts by weight. If the amount is less than 20 parts by weight, the heat resistance and hot water resistance, which are the objectives of the present invention, will not be good. Moreover, if it exceeds 70 parts by weight, it is not preferable because the processability is greatly reduced. The polystyrene used in the present invention may be either rubber-reinforced polystyrene or non-rubber-reinforced polystyrene. As the rubber-reinforced polystyrene, so-called high-impact polystyrene, which is obtained by polymerizing styrene in the presence of rubber such as polybutadiene, styrene-butadiene copolymer, polyacrylic ester, and ethylene-propylene-ethylidene copolymer, is usually used. However, polystyrene, polybutadiene, styrene-butadiene copolymer, styrene-butadiene block copolymer and/or its hydrogenated product, ethylene-propylene copolymer, ethylene-propylene-ethylidene norbornene terpolymer, polybutene rubber, acrylonitrile-butadiene copolymer Combined, polyisoprene,
Rubber-like elastic bodies such as natural rubber and polyester elastomer may be used alone or in a mechanical mixture of two or more types. In addition, so-called styrene compounds such as orthomethylstyrene, paramethylstyrene, chlorostyrene, and ethylvinyltoluene may be included as a part of the components constituting the polystyrene in the present invention. Polystyrene is used in an amount of 60 parts by weight or less; if it exceeds 60 parts by weight, heat resistance decreases and it becomes easily swollen by organic solvents, etc., which is not preferable. Examples of the polyamide used in the present invention include nylon 6, nylon 66, nylon 610, nylon 11,
Nylon 12, a copolymer of trimethylhexamethylene diamine and terephthalic acid, and modified products thereof can be used alone or in combination of two or more. The polyamide is used in an amount of 5 to 70 parts by weight. If it is less than 5 parts by weight, oil resistance will not be good, and if it exceeds 70 parts by weight, heat resistance and impact strength will decrease, which is not preferable. The copolymer of styrene and α,β-unsaturated dicarboxylic acid anhydride and/or unsaturated dicarboxylic acid imidide used in the present invention is not a rubber-reinforced copolymer even if it is a non-rubber reinforced copolymer. It can be used even if The α,β-unsaturated dicarboxylic acid anhydride may be any anhydride as long as it can be copolymerized with styrene, such as maleic anhydride, chloromaleic anhydride, citraconic anhydride, butenylsuccinic anhydride, and tetrahydrophthalic anhydride. A copolymer of an unsaturated dicarboxylic acid with an imidide may be obtained by directly copolymerizing styrene and an imide, but a copolymer with a styrene anhydride may be reacted with ammonia and/or a primary amine. It can also be imidized.
In addition, as a constituent component, styrene and anhydride of α,β-unsaturated dicarboxylic acid and/or α,β
- Other monomers copolymerizable with imidized unsaturated dicarboxylic acids, such as methacrylic esters, acrylic esters, acrylic acid, methacrylic acid, vinyl cyanide compounds, and styrene compounds other than styrene, etc. Alternatively, two or more types may be introduced. To obtain the rubber reinforcement, polybutadiene, styrene-butadiene copolymer, hydrogenated styrene-butadiene copolymer, acrylonitrile-butadiene copolymer, ethylene-propylene copolymer, polyacrylic acid ester, polyisoprene, natural rubber, etc. The above monomers may be polymerized in the presence of a rubbery elastic material, or these rubbery elastic materials may be mechanically mixed. Examples of suitable copolymers include styrene maleic anhydride copolymer, styrene maleic anhydride-methyl methacrylate copolymer, styrene-maleimide copolymer, styrene-N phenylmaleimide copolymer, and rubbers thereof. Reinforcements can be given. The anhydride of styrene and α,β-unsaturated dicarboxylic acid and/or the imide of α,β-unsaturated dicarboxylic acid are used in an amount of 3 to 40 parts by weight. If the amount is less than 3 parts by weight, the final composition will not be in a good compatibility state, resulting in a brittle product that may cause peeling phenomena, which is not preferable. Moreover, if it exceeds 40 parts by weight, the molding processability of the final composition deteriorates, which is undesirable. The halogenated polystyrene used in the present invention can be widely used, ranging from low molecular weight ones called oligomers to infinite molecular weight ones with a three-dimensional structure. A styrenic monomer may be polymerized, or a styrene monomer may be polymerized and then halogenated, and one or more types can be used.

[Formula] (where R is hydrogen, halogen, lower alkyl,
halogenated lower alkyl, X ₁ to _{X 5} are vinyl, halogen, hydrogen, lower alkyl, or lower halogenated alkyl, and at least one of X ₁ to _{X 5} is a halogen) halogenated polystyrene Specific examples of the constituent monomers include chlorostyrene, bromostyrene, 2,6-dichlorostyrene, 2,6-dibromostyrene, 2,4,6-tribromostyrene,
2,4,6-trichlorostyrene, α-methyl-
Chlorostyrene, α-methyl-bromostyrene,
2,6-dichloro-4-methylstyrene, 2,6
-dibromo-4-methylstyrene, pentachlorostyrene, pentabromostyrene, 2,6-bromo-1,4-divinylbenzene, and the like.
A particularly preferred halogen is bromine. The amount of halogenated polystyrene added is determined depending on the target degree of flame retardancy, but usually polyphenylene ether resin, polystyrene, polyamide, styrene and anhydride of α,β-unsaturated dicarboxylic acid and/or α,β-unsaturated dicarboxylic acid, Resin composition consisting of a copolymer of β-unsaturated dicarboxylic acid with imidide
Add 3 to 40 parts by weight per 100 parts by weight. If the amount is less than 3 parts by weight, almost no flame retardant effect will be obtained, and if it exceeds 40 parts by weight, the effect will not increase. The antimony compound used in the present invention may be inorganic or
Can also be used organically. For example, antimony oxide, antimony chloride, antimony phosphate, KSb(OH) ₆ ,
Examples include NH ₄ SbF ₆ , SbS ₃ KSb tartrate, Sb caproate, Sb (OCH ₂ CH ₃ ) ₃ , Sb polymethylene glycolate, and triphenyl antimony. A particularly preferred antimony compound is antimony oxide. The amount of the antimony compound to be added is determined depending on the target degree of flame retardancy, but it is added in an amount of 0 to 20 parts by weight per 100 parts by weight of the resin composition whose main component is the above-mentioned polyphenylene ether resin. Even if more than 20 parts by weight is added, the effect will not further increase. Depending on the purpose, the composition of the present invention may contain conventionally known flame retardants such as inorganic flame retardants such as Al(OH) ₃ , organic flame retardants such as phosphoric acid esters, and melamine flame retardants. I can do it. The composition of the present invention may also contain conventionally known additives, such as polybutene, low molecular weight polyethylene, mineral oil, epoxidized soybean oil, polyethylene glycol, plasticizers such as fatty acid esters, phosphorous esters, hindered phenols, One or more stabilizers such as alkanolamines, acid amides, dithiocarbamic acid metal salts, inorganic sulfides, and metal oxides, various ultraviolet absorbers, colorants, mold release agents, etc. can be added. . Furthermore, a reinforcing filler can be added to the composition of the present invention, and a filler-containing composition having extremely high rigidity and heat resistance can be obtained. As the filler, glass fiber, carbon fiber, various metal fibers, various metal flakes, asbestos, wollastonite, calcium carbonate, talc, mica, zinc oxide, potassium titanate, titanium oxide, glass beads, etc. can be used. . The composition of the present invention is no exception to the fact that functions such as conductivity and electromagnetic shielding properties can be imparted by selecting a conductive filler such as carbon fiber as the filler. The method for obtaining the composition of the present invention includes an extruder,
A method of melting and mixing using a kneader, roll mixer, Banbury mixer, etc. is used. In the case of melt mixing, all the components may be mixed at the same time, or some components may be mixed in advance, and then the remaining components may be added and mixed. The present invention will be described below with reference to Examples, but the present invention is not limited to the following Examples. In the examples, parts indicate parts by weight. In addition, physical property values were measured by the following method. Heat resistance: JIS using 1/4″ thick injection molded test piece
-Heat distortion temperature (hereinafter abbreviated as HDT) was measured at a load of 18.6 Kg/cm ² in accordance with K7207. Workability: Melt flow rate (hereinafter abbreviated as MFR) was measured at 280°C and a load of 10 kg. Impact strength: using 1/8″ thick injection molded specimens
Notched Izo impact strength was measured according to ASTM-D-638 (measurement temperature: 23°C). Flammability: Using 1/16″ thick injection molded specimens,
A UL-94 vertical combustion test was conducted. Hot water resistance: Judgment was made based on the change in appearance of the Izot impact test specimen after immersing it in boiling water for 500 hours and the degree of decrease in Izot impact strength (retention rate % relative to the value before immersion). Bleed test: After leaving an injection molded specimen with a thickness of 1/8″ in a gear oven at 100°C for 500 hours,
The presence or absence of bleed-out on the surface of the test piece was observed. Corrosion resistance to metal: 1mm thick test piece for bleed test
After the brass plates were tightly attached and clamped together and left in a gear oven at 100°C for 500 hours, the presence or absence of changes in the contact surface of the brass plate with the test piece was observed. Oil resistance: The Izot impact test specimen was immersed in cyclohexane for 24 hours, and was judged based on the change in appearance of the specimen and the degree of decrease in Izot impact strength (retention rate % relative to the value before immersion). Further, the raw materials used in this example are as follows. Polyphenylene ether: poly(2,6-dimethylphenylene-1,4-ether) with ηsp/c=0.60 (5% chloroform solution). (below
(abbreviated as PPE) Styron QH405: High impact polystyrene Styron 685, manufactured by Asahi Kasei Industries, Ltd.: Polystyrene Dylark #232, manufactured by Asahi Kasei Industries, Ltd.: Styrene-maleic anhydride copolymer manufactured by ARCO Polymers (maleic anhydride content: 10 %) Dilarc #332: Same as above (maleic anhydride content 15
%) Dylarc #250: Rubber reinforced styrene-maleic anhydride copolymer, manufactured by ARCO Polymer Co., Ltd. Styrene-N-phenylmaleimide copolymer: N
-Prototype polymerization of 10% phenyl-maleimide was used (hereinafter abbreviated as SPMI) Amiran #1017: Nylon 6 manufactured by Toray Industries, Inc. Leona 1300S: Nylon 66 manufactured by Asahi Kasei Corporation KRATON-G1650: SHELL Hydrogenated styrene-butadiene block copolymer Toughprene manufactured by Asahi Kasei Corporation: Styrene-butadiene block copolymer Pyrocheck 68PB manufactured by Nissan Ferro Organic Chemical Co., Ltd.: Poly(2,4,6-tribromostyrene) EB manufactured by Nissan Ferro Organic Chemical Co., Ltd. -800: Brominated cross-linked polystyrene manufactured by Matsunaga Chemical Co., Ltd. Decabro: Decabromodiphenyl ether Norbalett 120 manufactured by Matsunaga Chemical Co., Ltd.: Red phosphorus antimony trioxide sumilizer BHT manufactured by Rin Kagaku Kogyo Co., Ltd.: Sumitomo Chemical 2,6-ditertiarybutyl-4-methylphenol manufactured by Co., Ltd. (Example 1) 30 parts of PPE, 20 parts of Styron QH405, 10 parts of Styron 685, 10 parts of Dilarc #232, 30 parts of Amilan #1017, 12 parts of Pyrocheck 68PB 3 parts of antimony trioxide were uniformly mixed in a drum blender, and extrusion granulation was performed at 280°C using a 30 mm twin-screw extruder to obtain composition pellets. This is 5
Injection molded at 280℃ using an ounce injection molding machine,
A test piece was obtained and subjected to a test, and the following results were obtained. HDT 115°C, MFR 6.2 g/10 minutes, Izod impact strength 18 Kg/cm, flame retardancy rank V-1. Furthermore, after 500 hours of immersion in boiling water, no changes were observed on the surface of the test piece, and the Izot impact strength was 16.2.
It showed a high value of Kg・cm/cm (retention rate 90%). Furthermore, even after being subjected to an oil resistance test using cyclohexane, no changes such as crack-induced swelling or moisture were observed on the surface of the test piece, and the Izot impact strength was 17.3.
It showed a high value of Kg・cm/cm (retention rate 96%). In addition, the test piece was placed in a gear oven at 100°C for 500 min.
After leaving it for a while, the surface of the test piece was observed, but no change was observed. In addition, a brass board was fixed to the test piece, and after leaving it in a gear oven at 100° C. for 500 hours, the surface of the brass board was observed, but no changes such as discoloration were observed. (Example 2) 60 parts of PPE, 10 parts of Styron QH405, 10 parts of Dilarc #232, 20 parts of Amilan #1017, 12 parts of Pyrocheck 68PB, and 3 parts of antimony trioxide were extruded and granulated by the method of Example 1, and molded. It was subjected to a post-test. The result is as follows. HDT 144℃, MFR 2.0g/10 minutes, Izotsu impact strength 21Kg・cm/cm Flame retardant rank V-1, Hot water test: No change on the test piece surface, Izotsu impact strength 20.5Kg・cm/cm (retention rate 98%), oil resistance test:
No change on test piece surface, Izotsu impact strength 18.4
Kg・cm/cm (retention rate 92%), Bleed test: No change, Metal corrosion test: No change on the brass plate surface (Example 3) In Example 1, Pyro-checked Die-Lark #232 to Die-Lark #332 68PB was replaced with EB800 and subjected to the same evaluation as in Example 1, and the results shown in Table 1 were obtained. (Example 4) In Example 1, Dilarc #232 was replaced with Dilarc #250 and Pyrocheck 68PB was replaced with EB800, and the same tests as in Example 1 were conducted, and the results shown in Table 1 were obtained. (Example 5) In Example 1, Amiran #1017 was replaced with Leona.
1300S and subjected to the same test as in Example 1, and the results shown in Table 1 were obtained. (Example 6) 30 parts of PPE, 17 parts of Dilarc #232, 50 parts of Amilan #1017, 3 parts of KRATON1650, 35 parts of Pyrocheck 68PB, and 10 parts of antimony trioxide were extruded and granulated in the same manner as in Example 1 and molded. A post-test was conducted and the results shown in Table 2 were obtained. (Example 7) 30 parts of PPE, 2 parts of Styron QH405, 35 parts of Dilarc #232, 30 parts of Amiran #1017,
KRATON1650 Part 3, Pyrocheck 68PB12
3 parts of antimony trioxide were extruded and granulated in the same manner as in Example 1, molded, and then subjected to testing.
The results were obtained. (Example 8) In Example 1, 12 copies of Pyrocheck 68PB,
Pyrocheck 3 parts of antimony trioxide 68PB 35
and subjected to the same test as in Example 1.
2 results were obtained. (Example 9) 60 copies of PPE, 12 copies of QH405, Dailarc #232 5
part, Amilan #1017 10 parts, Tuffprene 3 parts, Pyrocheck 68PB 7 parts, Antimony trioxide 5 parts,
0.1 part of Sumilizer BHT was extruded and granulated in the same manner as in Example 1, molded, and then subjected to a test.
2 results were obtained. (Example 10) In Example 1, Dailarc #232 was connected to SPMI
The test was performed in the same manner as in Example 1, and the results shown in Table 2 were obtained. (Example 11) 40 parts of PPE, 15 parts of Styron 685, 15 parts of Dilarc #232, 30 parts of Amilan #1017, Pyrocheck 68PB, and 3 parts of antimony trioxide were extruded and granulated in the same manner as in Example 1, and then molded. It was subjected to a test and the results shown in Table 2 were obtained. (Comparative Example 1) 75 parts of PPE, 5 parts of Dilarc #232, 20 parts of Amilan #1017, 12 parts of Pyrocheck 68PB, and 3 parts of antimony trioxide were extrusion granulated by the method of Example 1, and the MFR of the resulting composition was Measured at 0.4
The value was extremely low at g/10 minutes. (Comparative Example 2) In Example 1, 30 parts of PPE, 30 parts of Amilan #1017
10 parts of PPE and Amilan #1017 were used for the test, and the results are shown in Table 3. That is, the HDT was extremely low at 70°C, and the test piece subjected to the hot water resistance test was deformed. (Comparative Example 3) In Example 1, 20 parts of Styron QH405 and 10 parts of Dilarc #232 were replaced with 28 parts of Styron QH405,
Dilarc #232 2 parts replaced for test -
3 results were obtained. Izotsu impact strength is 5.2Kg・
Only a low value of cm/cm was obtained, and a peeling phenomenon was observed on the fracture surface of the test piece. (Comparative Example 4) In Example 1, 12 parts of Pyrocheck 68PB and 3 parts of antimony trioxide were replaced with 2 parts of Pyrocheck, and the results shown in Table 3 were obtained. A flame retardant composition could not be obtained. (Comparative Example 5) In Example 1, 20 parts of Styron QH405, 10 parts of Styron 685, 10 parts of Dilarc #232, and 30 parts of Amilan #1017 were placed in 45 parts of Dilarc #232, 20 parts of Amilan #1017, and 5 parts of KRATON1650. Instead, when the MFR of the composition obtained by extrusion granulation by the method of Example 1 was measured, it was an extremely low value of 0.7 g/10 minutes. (Comparative Example 6) In Example 1, 20 parts of QH405 and 30 parts of Amilan #1017 were replaced with 46 parts of Styron QH405 and 4 parts of Amilan #1017, and the results were subjected to the test. Table 4
The results were obtained. Cracks occurred in the test piece subjected to the oil resistance test, and the Izot impact strength of the test piece also significantly decreased to 10.8 Kg·cm/cm (retention rate 57%). (Comparative Example 7) In Example 1, 12 parts of Pyrocheck was replaced with 12 parts of Dekabro and the test pieces were used to obtain the results shown in Table 4. The surface of the test piece used in the bleed test turned white due to white fine powder, which could be removed by rubbing with fingers. In addition, the surface of the brass plate used in the metal corrosion test that was in close contact with the resin was discolored to a black spot. (Comparative Example 8) In Example 1, Pyrocheck 68PB 12
120 parts, 3 parts of antimony trioxide
The results shown in Table 4 were obtained.
Many fine bulges were generated on the surface of the test piece subjected to the hot water resistance test, and the Izod impact strength of the test piece was significantly reduced to 8.4 Kg cm/cm (retention rate 56%). . (Comparative Example 9) 15 parts of PPE, 5 parts of Dilarc #232, 80 parts of Amilan #1017, 12 parts of Pyrocheck 68PB, and 3 parts of antimony trioxide were extruded and granulated by the method of Example 1, and subjected to a test. Got the results. HDT
The temperature was as low as 80°C, and the Izot impact strength was extremely low at 3.0. In addition, the test piece used for the hot water resistance test was deformed.

【table】

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【table】

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Claims (1)

[Claims] 1 (a) Polyphenylene ether resin
20 to 70 parts by weight (b) Polystyrene 0 to 60 parts by weight (c) Polyamide 5 to 70 parts by weight (d) Anhydride of styrene and α,β-unsaturated dicarboxylic acid and/or α,β-unsaturated dicarboxylic acid For 100 parts by weight of a resin composition consisting of 3 to 40 parts by weight of a copolymer with an imidide of (e) 3 to 40 parts by weight of halogenated polystyrene having a structure obtained by polymerizing monomers of the following general formula [ Formula] (where R is hydrogen, lower alkyl, halogen or halogenated lower alkyl,
X ₁ to X ₅ are vinyl, halogen, hydrogen, lower alkyl halide, or lower alkyl, and at least one of X ₁ to _{X 5} is a halogen) (f) Antimony-containing compound 0 to 20 by weight Composition 2 Polyphenylene ether resin is selected from polymers having repeating units represented by the following general formula [Formula] (However, R ₁ and R ₂ are the same or different tert- Alkyl group having 1 to 4 carbon atoms excluding butyl group, aryl group,
The composition according to claim 1, which is a halogen atom or a hydrogen atom). 3. The composition according to claim 1, wherein the polyphenylene ether is poly(2,6-dimethyl-1,4-phenylene) ether. 4. The anhydride of α,β-unsaturated dicarboxylic acid is maleic anhydride. Composition 5 according to Claim 1, wherein the imidized product of α,β-unsaturated dicarboxylic acid is N-phenylmaleimide Composition 6 according to Claim 1, wherein the halogen is bromine A composition according to claim 1.