JPH08199014A - Thermoplastic resin composition - Google Patents

Abstract

PURPOSE: To obtain a thermoplastic resin composition improved in heat resistance and film adhesion without detriment to excellent impact resistance and flexibility inherent in the constituent ethylene/α,β-unsaturated carboxylic acid ester copolymer. CONSTITUTION: This composition comprises 100 pts.wt. component containing 40-99wt.% ethylene/α,β-unsaturated carboxylic acid ester copolymer and 1-60wt.% polyphenylene ether and 1-50 pts.wt. epoxy group containing ethylene copolymer.

Description

Detailed Description of the Invention

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a thermoplastic resin composition containing a copolymer of ethylene and an α, β-unsaturated carboxylic acid ester, a polyphenylene ether and an epoxy group-containing ethylene copolymer as essential components. Specifically, the present invention has improved the heat resistance and coating adhesion thereof without impairing the excellent impact resistance and flexibility possessed by the copolymer of ethylene and α, β-unsaturated carboxylic acid ester. It relates to a thermoplastic resin composition.

[0002]

2. Description of the Related Art Copolymers of ethylene and α, β-unsaturated carboxylic acid esters have excellent impact resistance, flexibility,
Utilizing high temperature processability, low odor, weather resistance, flexibility, etc.,
It is used for extrusion lamination, wire coating, and various sheets and films.

[0003]

However, an injection molded article of a copolymer of ethylene and an α, β-unsaturated carboxylic acid ester, for example, impact resistance and flexibility of an automobile exterior material such as a side molding or a mudguard is used. The injection-molded article, which is required to have heat resistance, heat resistance, and coating film adhesion at the time of coating, has a problem of insufficient heat resistance and coating film adhesion.
However, in order to improve the heat resistance of the copolymer of ethylene and α, β-unsaturated carboxylic acid ester, when a polyolefin such as polypropylene is blended with the copolymer, the heat resistance of the resulting blend is improved. Is improved, but the coating adhesion is worse than that of the copolymer. The object of the present invention is to improve the heat resistance and coating adhesion of an α, β-unsaturated carboxylic acid ester copolymer without impairing the excellent impact resistance and flexibility of the copolymer. It is to provide a thermoplastic resin composition.

[0004]

DISCLOSURE OF THE INVENTION The inventors of the present invention have found that the heat resistance of ethylene and α, β-unsaturated carboxylic acid ester without compromising the excellent impact resistance and flexibility possessed by the copolymer. And, intensive research has been conducted to develop a thermoplastic resin composition having improved coating film adhesion. As a result, a thermoplastic resin composition prepared by blending a copolymer of ethylene and an α, β-unsaturated carunsaturated carboxylic acid ester with a polyphenylene ether and an epoxy group-containing ethylene copolymer is ethylene and α, β- The inventors have found that the heat resistance and the coating film adhesion are improved without impairing the excellent impact resistance and flexibility of the copolymer with the unsaturated carboxylic acid ester, and the present invention has been completed. . That is, the present invention is a copolymer of ethylene and α, β-unsaturated carboxylic acid ester (hereinafter, also referred to as “component (A)”) 40 to 99.
% By weight and 100 parts by weight of a component containing 1 to 60% by weight of polyphenylene ether (hereinafter, also referred to as “component (B)”) and an epoxy group-containing ethylene copolymer (hereinafter,
A thermoplastic resin composition containing 1 to 50 parts by weight of "component (C)".

Α related to the component (A) used in the present invention,
As β-unsaturated carboxylic acid ester, ethyl acrylate, methyl acrylate, 2-ethyl acrylate,
Examples thereof include acrylic acid esters such as stearyl acrylate, and methacrylic acid esters such as methyl methacrylate, ethyl methacrylate, 2-ethylhexyl methacrylate, and stearyl methacrylate.

Examples of the preferred component (A) used in the present invention include a copolymer of ethylene and ethyl acrylate, a copolymer of ethylene and methyl acrylate, and a copolymer of ethylene and methyl methacrylate.

The component (A) can be produced from ethylene and an α, β-unsaturated carboxylic acid ester by a known polymerization method, or a known copolymer as the component (A) can be used.

Α and β in the component (A) used in the present invention
The content of repeating units derived from unsaturated carboxylic acid ester is 3 to 60% by weight, preferably 5 to 40% by weight. When the content of the repeating unit is less than 3% by weight, the coating film adhesion of the composition of the present invention is insufficient, and when the content is more than 60% by weight, the composition of the present invention is Insufficient heat resistance.

The melt index of the component (A) used in the present invention is 0.2 to 400 g / 10 minutes (measurement method is AS
(TM I-1238, 190 ° C) is preferred.

The component (B) used in the present invention is a known polymer, and one or two or more of the phenol compounds represented by the general formula 1 are treated with oxygen or an oxygen-containing gas using an oxidative coupling catalyst. It is a polymer obtained by oxidative polymerization.

[0011]

Embedded image (In the formula, R ₁ , R ₂ , R ₃ , R ₄ and R ₅ are selected from hydrogen, a halogen atom, a hydrocarbon group or a substituted hydrocarbon group, and one of them is always a hydrogen atom)

R ₁ , R ₂ , R ₃ , R in the general formula 1
Specific examples of ₄ and R ₅ are hydrogen, chlorine, bromine, fluorine, iodine, methyl, ethyl, n- or iso-propyl, pri-, sec- or t-butyl, chloroethyl, hydroxyethyl, phenylethyl, benzyl. , Hydroxymethyl, carboxyethyl, methoxycarbonylethyl, cyanoethyl, phenyl, chlorophenyl, methylphenyl, dimethylphenyl, ethylphenyl and allyl.

Specific examples of the general formula 1 include 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, 2-
Methyl-6-allylphenol may be mentioned.

Further, a phenol compound other than the one represented by the general formula 1 such as bisphenol-A, tetrabromobisphenol-A, resorcin, hydroquinone, a polyhydric aromatic compound such as novolac resin and the general formula 1
Copolymers with and can also be used as component (B).

As the preferred component (B) used in the present invention, a homopolymer of 2,6-dimethylphenol or 2,6-diphenylphenol, a large amount of 2,6-xylenol and a small amount of 3-methyl-. A copolymer with 6-t-butylphenol or 2,3,6-trimethylphenol is exemplified. Further, the intrinsic viscosity η ₀ of the component (B) is 0.45 or less, preferably 0.4 or less.

The oxidative coupling catalyst used in the oxidative polymerization of the phenol compound is not particularly limited, and any catalyst having a polymerization ability can be used.

The mixing ratio of the component (A) and the component (B) used in the production of the composition of the present invention is 40 to 40% of the component (A).
It is 99% by weight and 1 to 60% by weight of the component (B), and the total amount of both components is 100% by weight.

The component (C) used in the present invention is an epoxy group-containing ethylene copolymer having an epoxy group in the main chain or side chain. The copolymer is obtained by copolymerizing ethylene and a monomer having an epoxy group, or by oxidizing the carbon-carbon double bond in the copolymer of ethylene and a diene compound such as butadiene with ozone or the like. can get. The component (C) is preferably a unit derived from ethylene (hereinafter, also referred to as “unit (a)”) and a unit derived from an unsaturated carboxylic acid glycidyl ester copolymerizable with ethylene (hereinafter, “unit”). (B-1) ") or a unit derived from glycidyl ether having an unsaturated group copolymerizable with ethylene (hereinafter," unit (b
-2) ") is also included as an essential repeating unit.

The unsaturated carboxylic acid glycidyl ester which induces the unit (b-1) is a compound represented by the general formula 2.

[0020]

Embedded image (In the formula, R is 2 to 2 carbon atoms having an ethylenically unsaturated bond.
18 alkenyl groups)

Examples of the compound represented by the general formula 2 include glycidyl acrylate, glycidyl methacrylate, and itaconic acid glycidyl ester.

The glycidyl ether having an unsaturated group which induces the unit (b-2) is a compound represented by the general formula 3.

[0023]

Embedded image (In the formula, R is 2 to 2 carbon atoms having an ethylenically unsaturated bond.
18 is an alkenyl group, and X is CH ₂ —O or O)

Examples of the compound represented by the general formula 3 include allyl glycidyl ether, 2-methylallyl glycidyl ether and styrene-p-glycidyl ether.

The component (C) comprises a unit (a) and a unit (b-
In addition to 1) or (b-2), a unit derived from an ethylenically unsaturated compound (hereinafter, also referred to as "unit (c)")
Can be included as any repeating unit.

Examples of the ethylenically unsaturated compound for deriving the unit (c) include α, β-unsaturated carboxylic acid alkyl esters such as methyl acrylate, ethyl acrylate, butyl acrylate and methyl methacrylate, vinyl acetate, vinyl propionate and butanoic acid. Examples thereof include carboxylic acid vinyl esters such as vinyl, vinyl ethers such as methyl vinyl ether, ethyl vinyl ether, propyl vinyl ether and phenyl vinyl ether, and styrenes such as styrene, methylstyrene and ethylstyrene.

The composition ratio of each unit constituting the component (C) is 50 to 99% by weight of the unit (a), and 0.1 to the unit (b).
It is 50% by weight, preferably 0.5 to 20% by weight, and the unit (c) is 0 to 50% by weight, preferably 10 to 40% by weight.

Specific examples of the component (C) include ethylene-glycidyl methacrylate copolymer, ethylene-glycidyl methacrylate-methyl acrylate copolymer, ethylene-glycidyl methacrylate-ethyl acrylate copolymer, ethylene-glycidyl methacrylate-vinyl acetate. A copolymer is mentioned. Among them, ethylene-glycidyl methacrylate copolymer, ethylene-glycidyl methacrylate-methyl acrylate copolymer, and ethylene-glycidyl methacrylate-ethyl acrylate copolymer are preferable.

The glycidyl group content of component (C) is 0.1
It is preferable that the content of the component (C) is 0.5 to 3000 g / 10 minutes (J
ISK6760) is preferred.

The component (C) can be produced by various known polymerization methods. For example, a method of copolymerizing ethylene and a compound represented by general formula 2, a method of copolymerizing ethylene and a compound represented by general formula 3, ethylene, a compound represented by general formula 2 and a general formula In general, a method of copolymerizing with the compound represented by 3 or a homopolymer of ethylene or a copolymer of ethylene with an olefin such as propylene copolymerizable with ethylene (hereinafter, also referred to as "ethylene-based copolymer") A method of graft-polymerizing the compound represented by the formula 2 or 3, and a copolymer of ethylene and an ethylenically unsaturated compound which derives the unit (c) with the compound represented by the formula 2 or 3. The method of making it possible can be illustrated.

As a specific example of the method for producing the component (C), ethylene and the compound represented by the general formula 2 or 3 are added in the presence of a radical generator under a pressure of 500 to 4000 atm to 100 to 300. A method of copolymerizing at a temperature of ℃ in the presence or absence of a suitable solvent or chain transfer agent,
The ethylene-based copolymer, which is a homopolymer of ethylene or a copolymer of ethylene and propylene, has the general formula 2 or 3
A method of mixing the compound represented by and a radical generator, and melt-kneading the mixture in a Banbury kneader or an extruder to perform graft copolymerization can be exemplified.

The composition of the present invention is a polymer of a monomer selected from the group consisting of olefins, diolefins and vinyl aromatic compounds in addition to the components (A), (B) and (C). A polymer having no ester or epoxy functional group (hereinafter, also referred to as “component (D)”) can be included.

As the polymer as the component (D), for example, ethylene, propylene, butene-1, pentene-1, 4-methylpentene-1, isobutylene, 1,4-hexadiene, dicyclopentadiene, 2,5-norbornadiene, 5-ethylidene norbornene, 5-ethyl-2,5
-Norbornadiene, 5- (1'-propenyl) -2-
Examples thereof include polymers of at least one monomer selected from norbornene and styrene. Examples of preferred component (D) include polyethylene and polypropylene, as well as block or random copolymers of α-olefins such as ethylene, propylene and butene.

The mixing ratio of the component (D) is 1 to 200 parts by weight based on 100 parts by weight of the total amount of the components (A) and (B). When the blending ratio of the component (D) exceeds 200 parts by weight, the resulting composition has insufficient impact resistance and coating film adhesion.

The composition of the present invention may contain various fillers in order to improve rigidity, hardness and the like as required. Examples of the filler include calcium carbonate, magnesium carbonate, aluminum hydroxide, magnesium hydroxide, zinc oxide, titanium oxide, magnesium oxide, aluminum silicate, magnesium silicate, calcium silicate, silicic acid, hydrous calcium silicate, hydrous silicic acid. Aluminum acid,
Mica, mineral fiber, xonotlite, potassium titanate
Examples include whiskers, magnesium oxysulfate, glass balun, glass fibers, glass beads, carbon fibers, inorganic fibers such as stainless fibers, aramid fibers, and carbon black, and the composition of the present invention may contain one or more of these fillers. .

The compositions of the present invention may also contain various additives such as flame retardants, plasticizers, antioxidants, weathering agents. In particular, when an additive known as an additive of the component (A), the component (B) or the component (D) is used, the physical properties of the resulting composition may be further improved.

The thermoplastic resin composition of the present invention can be produced by melt-kneading the components to be used by a known method. The order in which the components are mixed and the order in which the components are melt-kneaded in the melt-kneading are arbitrary. For example, a method in which all the components are blended together and then the mixture is melt-kneaded, and some of the components and their components are used. A method in which the remaining components are separately blended and melt-kneaded, and then the obtained plurality of kneaded products are collectively melt-kneaded, and a plurality of feed ports are provided from the upstream side to the downstream side of the extruder. In one extruder, a method of sequentially feeding each component from each feed port and melt-kneading in the extruder can be exemplified. As a preferable melt-kneading method, the component (B), the component (C) and the component (D) are fed from the upstream feed port of the extruder having two feed ports, and the component (A) is fed from the downstream feed port. The melt-kneading method of feeding the can be exemplified.

The thermoplastic resin composition of the present invention can be easily molded by a molding method generally applied to a thermoplastic resin or a resin composition, that is, an injection molding method, an extrusion molding method, a hollow molding method or the like. You can Since the composition of the present invention has good impact resistance, flexibility, heat resistance, coating adhesion, etc., it is suitable for use as an injection molded product such as a side molding, a mudguard, a bumper, or a vehicle part such as a window frame. obtain.

The composition of the present invention has a morphology in which the component (A) is the continuous phase and the component (B) is the dispersed phase. In order to achieve the object of the present invention, the dispersed phase particles of the component (B) are used. The diameter is preferably 5 μm or less.

[0040]

In the present invention, the component (B) is used to improve heat resistance and coating adhesion, and the component (D) is used to improve heat resistance and impact resistance. How the component (C) works in the composition,
The mechanism of action itself is not clear. However, (B) in the composition obtained by melt-kneading the component (A) and the component (B), which have originally low compatibility, in the absence of the component (C).
Has a large dispersed particle size of 10 μm or more, and the mechanical properties of the composition are extremely low, while surprisingly, when both components are melt-kneaded in the presence of the component (C). The dispersed particle size of (B) in the composition obtained in (1) is smaller than that, and the mechanical properties of the composition are extremely good. Therefore, it is presumed that, as a result of the component (C) improving the compatibility between the component (A) and the component (B), the dispersibility of the (B) in the resulting composition is improved.

[0041]

EXAMPLES Examples of the present invention will be shown below, but the present invention is not limited thereto. The components used are as follows.

Component (A) Polymer-A: a copolymer of ethylene and methyl methacrylate having a methyl methacrylate content of 5
% By weight, melt index 2 (190 ° C., 216
(kg load). Polymer-B: a copolymer of ethylene and methyl methacrylate, having a methyl methacrylate content of 2
0% by weight, melt index 20 (190 ° C, 2.
16 kg load). Polymer-C: a copolymer of ethylene and methyl methacrylate, having a methyl methacrylate content of 2
0% by weight, melt index 70 (190 ° C, 2.
16 kg load). Polymer-D: a copolymer of ethylene and ethyl acrylate, having an ethyl acrylate content of 20% by weight and a melt index of 20 (190 ° C, 2.16).
(kg load).

Component (B) A chloroform solution (concentration: 0.5 g / d ) obtained by homopolymerizing 2,6-dimethylphenol.
l), polyphenylene ether having an inherent viscosity of 0.30 at 30 ° C. Hereinafter, the polyphenylene ether is referred to as "PP
Also called "E".

Component (C) EPO-1: a copolymer of ethylene and glycidyl methacrylate having a glycidyl methacrylate content of 6
Wt%, melt index 3 (190 ° C, 2.16
(kg load). EPO-2: a copolymer of ethylene, glycidyl methacrylate and methyl acrylate, having a glycidyl methacrylate content of 3% by weight, a methyl acrylate content of 30% by weight and a melt index of 9 (190 ° C,
2.16 kg load). EPO-3: a copolymer of ethylene, glycidyl methacrylate and methyl acrylate, having a glycidyl methacrylate content of 6% by weight, a methyl acrylate content of 30% by weight and a melt index of 20 (190 ° C.,
2.16 kg load).

Component (D) BPP: ethylene-propylene part 30 wt%, block polypropylene, having a melt index of 8d.
g / min (230 ° C, 2.16 kg load) EPR: ethylene-propylene rubber obtained by polymerization of ethylene and propylene, having an ethylene content of 22% by weight and a melt index of 0.9 dg / min (19
0 ° C, 2.16 kg load).

Examples 1 to 7 The mixing ratio (parts by weight) of each component is as shown in Tables 1 and 2. Component (B) and component (C), or component (B), component (C) and component (D), the first on the upstream side of the twin-screw kneading extruder (TEM50 manufactured by Toshiba Machine Co., Ltd.). After being charged from the feed port and melted and kneaded at a cylinder temperature of 260 ° C., the component (A) is charged from the second feed port on the downstream side provided between the first feed port and the die and fed from the upstream side. The obtained melt-kneaded product and the component (A) were melt-kneaded. Cylinder temperature on the downstream side from the second feeder port is 20
It was set to 0 ° C. The molten resin extruded from the die was cooled in a water tank and then pelletized by a strand cutter.

Comparative Examples 1-3 Comparative Example 1 is the same as Example 1 except that the component (C) is not used.
This is an example performed in the same manner as. Comparative Examples 2 and 3 are the components (B)
This is an example performed in the same manner as in Example 2 except that the component (C) is not used.

The method of preparing the test piece and the test method are as follows. That is, the obtained pellets are vacuum dried at a temperature of 60 ° C. for 3 hours, and then the injection molding machine (Toshiba Machine IS
220 EN), a flat plate having a thickness of 3.0 mm was formed from the pellets under the conditions of a cylinder temperature of 200 ° C., an injection pressure of 1200 kg / cm ² , and a mold temperature of 30 ° C.

Melt Index (hereinafter, also referred to as "MI". The unit is dg / min) After vacuum drying the above pellets at a temperature of 60 ° C. for 3 hours,
It was determined by measurement under the conditions of 230 ° C. and a load of 2.16 kg.

Izod impact strength (unit: kgfcm /
cm) A flat plate having a thickness of 3.0 mm is cut to prepare a test piece (with a notch) for an Izod impact test, and ASTM D256
The test was conducted in an atmosphere of −30 ° C.

Flexural Modulus (Unit: kgf / cm ² ) The above-mentioned flat plate having a thickness of 3.0 mm was cut to prepare a test piece for a bending test, which was tested in an atmosphere of 23 ° C.

Heat Sag (Unit: mm) 125 made by cutting the above flat plate having a thickness of 3.0 mm
One end of a mm × 25 mm × 3.0 mm (thickness) test piece was fixed with an overhang of 100 mm, left at 90 ° C. for 1 hour, and then left at 23 ° C. for 1 hour, and the tip portion The amount of deformation due to the thermal history of (the amount that was lowered compared to before the test) was measured.

Coating adhesion 150 made by cutting the above-mentioned flat plate having a thickness of 3.0 mm
After coating a coating of Recolac # 2300 (manufactured by Fujikura Kasei Co., Ltd.) on a test piece of mm × 150 mm × 3 mm (thickness) under a normal condition with a coating gun to a thickness of about 25 to 30 μm, Dried in oven for 30 minutes at 80 ° C. A cellotape peeling test was performed on the test pieces that had been dried for 24 hours and 48 hours. Here, the cellotape peeling test is as follows. That is, first, by using a knife to make parallel line notches having a width of about 2 mm in the vertical and horizontal directions on the coating surface of the test piece,
10 grids about 2mm x 2mm on the surface of the coating film
Create 0. After that, a cellophane tape is pasted on the grid. After that, the cellophane tape was peeled off, and the remaining rate of the coating film that was not peeled off (remaining rate per 100 grids)
To measure. The larger the residual rate, the greater the coating film adhesion.

Dispersion particle size of polyphenylene ether (unit: μm) After cooling the flat plate having a thickness of 3.0 mm with liquid nitrogen,
An ultrathin section was prepared from the plate with a microtome at 80 ° C., stained with ruthenium oxide (RuO ₄ ), and observed with a transmission electron microscope to determine the number average dispersed particle size of polyphenylene ether.

Regarding Examples 1 to 5, Table 1 and Examples 6 to
7 and Comparative Examples 1 to 3 are summarized in Table 2.

[0056]

INDUSTRIAL APPLICABILITY According to the present invention, by dispersing and stabilizing polyphenylene ether by using an epoxy group-containing ethylene copolymer in a copolymer of ethylene and an α, β-unsaturated carboxylic acid ester, ethylene and α, A resin composition having improved heat resistance and coating adhesion without impairing the excellent impact resistance and flexibility possessed by the copolymer with β-unsaturated carboxylic acid ester can be obtained.

[0057]

[Table 1] ──────────────────────────────────── Example 1 Example 2 Example 3 Implementation Example 4 Example 5 ───────────────────────────────────── Ingredient (A) Polymer-A 70 − − − 50 Polymer-B − − 30 − − Polymer-C − 30 − − − Polymer-D − − − 30 −Ingredient (B) PPE 15 15 15 15 15 15Ingredient (C) EPO-2-10 10 10 15 EPO-3 15 -----Ingredient (D) BPP-35 35 35 35 20 EPR-10 10 10 10 10 ──────────────────────────────────── MI 3 15 11 11 4 Izod impact strength 4.7 6.2 6.2 6.5 6.6 9.1 Flexural modulus 2300 3500 3600 3400 1900 Heat sag 3.2 4.2 2.1 2.2 4.9 Coating adhesion After 24 hours 75 95 75 75 81 85 48 After 48 hours 99 100 99 99 99 99 PPE dispersed particle size 2.3 − − − − − ───────────────────── ────────────────

[0058]

[Table 2] ──────────────────────────────────── Example 6 Example 7 Comparative Example 1 Comparative Example 1 Example 2 Comparative Example 3 ──────────────────────────────────── Ingredient (A) Polymer-A − − 82.4 − − Polymer-C 30 30 − 45 33Ingredient (B) PPE 15 20 17.6-17Ingredient (C) EPO-1 10 − − − − EPO-2 − − − 10 − EPO-3 − 10 − − −Ingredient (D) BPP 35 30-35 39 EPR 10 10-10 10 11 ──────────────────────────────────── MI 12 12 6 35 22 Izod impact strength 5.5 6.3 1.3 1.3 13 1.7 Flexural modulus 4100 3500 4100 2600 3900 Heat sag 1.8 3.8 3.0> 508Coating adhesion After 24 hours 65 98 11 82 72 72 After 48 hours 98 100 29 29 93 86 PPE dispersed particle size −1.9 12 − − ───────────────────── ────────────────

Claims (4)

[Claims] 1. 100 parts by weight of a component (A) a copolymer of ethylene and an α, β-unsaturated carboxylic acid ester (40 to 99% by weight) and component (B) a polyphenylene ether (1 to 60% by weight), and a component. (C) A thermoplastic resin composition containing 1 to 50 parts by weight of an epoxy group-containing ethylene copolymer. 2. An epoxy group-containing ethylene copolymer as the component (C) is a unit 50-99 derived from ethylene (a).
% By weight, (b-1) units derived from unsaturated carboxylic acid glycidyl ester copolymerizable with ethylene or (b
-2) Epoxy containing 0.1 to 50% by weight of a unit derived from glycidyl ether having an unsaturated group copolymerizable with ethylene and (c) 0 to 50% by weight of a unit derived from an ethylenically unsaturated compound. The thermoplastic resin composition according to claim 1, which is a group-containing ethylene copolymer. 3. A total amount 1 of the components (A), (B) and (C).
Polymers 1 to 200, which are polymers of monomers selected from the group consisting of olefins, diolefins and vinyl aromatic compounds (D) and have no ester or epoxy functional groups per 100 parts by weight. The thermoplastic resin composition according to claim 1, comprising parts by weight. 4. The thermoplastic resin composition according to claim 1, wherein the dispersed particle diameter of the component (B) polyphenylene ether is 5 μm or less.