JPH0841278A - Resin composition - Google Patents

Abstract

PURPOSE:To obtain a polypropylene-based resin composition combinedly providing excellent impact resistance, heat resistance and tensile properties and excellent in a balance of physical properties. CONSTITUTION:This composition is constituted so as to have a polymer component containing a polypropylene-based polymer having at least a propylene- ethylene block copolymer and an ethylene-butene-based rubber and a polyethylene-ethylene/propylene-polyethylene triblock copolymer therein, and in fractionation by xylene, a ratio of a component soluble in 70 deg.C xylene is 25-60 pts.wt. and interfacial strength of a plane interface between (A) a component of a polypropylene-based polymer soluble in 90 deg.C xylene and (B) a component insoluble in 110 deg.C xylene is 20-500 (J/m<2>) when the interfacial strength is measured at a phase angle in a range from -2 deg. to -12 deg. by an asymmetric double cantilever beam method.

Description

Detailed Description of the Invention

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a resin composition having excellent impact resistance and rigidity and high heat resistance.
For example, the present invention relates to a resin composition suitable as a material for automobile bumpers, automobile interior and exterior parts, and the like.

[0002]

BACKGROUND OF THE INVENTION As a material for automobile bumpers and interior / exterior parts, a blend of polypropylene and ethylene-propylene rubber such as propylene homopolymer, propylene block copolymer, propylene random copolymer and the like has been conventionally used (Japanese Patent Publication No. Sho 60). No. 3420), a blend polymer of polypropylene, ethylene-propylene rubber, and ethylene-butene rubber (JP-A-4-372637).

[0003]

However, in the material composed of the blend polymer of polypropylene and ethylene-propylene rubber, the impact resistance is sufficient, but the heat resistance at the time of tensile is not sufficient. A material composed of a blend polymer of ethylene-propylene rubber and ethylene-butene rubber has improved heat resistance, but has a drawback of low impact resistance.

The present invention has been made in order to solve these problems, and an object thereof is to provide a polypropylene resin composition having excellent impact resistance, heat resistance and tensile strength, and having excellent physical property balance. It is what

[0005]

The first aspect of the present invention is to provide a polypropylene-based polymer having at least a propylene-ethylene block copolymer in its components, an ethylene-butene-based rubber, and a polyethylene-ethylene / propylene. -A polyethylene triblock copolymer and a polymer component containing it, and in the fractionation by xylene, the ratio of the component soluble in 70 ° C xylene is 25 to 60.
In parts by weight, the interfacial strength of a flat interface between the component (A) soluble in 90 ° C xylene and the component (B) insoluble in 110 ° C xylene of the polypropylene-based polymer is asymmetric double cantilever. Phase angle from -2 ° with beam method
20-500 (J / m when measured in the range of 12 °
² ) A resin composition characterized in that

A second aspect of the present invention is to provide a polypropylene polymer having at least a propylene-ethylene block copolymer in its components, an ethylene-butene rubber, and a polystyrene-ethylene / propylene-polyethylene triblock copolymer. And a polymer component containing a polymer, and the fraction soluble in 70 ° C xylene is 25 to 60 parts by weight in the fractionation with xylene. The interfacial strength of the flat interface between the soluble component (A) and the 110 ° C xylene-insoluble component (B) has a phase angle of −2 ° to −12 ° in the asymmetric double cantilever beam method. When measured, the resin composition is ^{20 to} 500 (J / m ² ).

At this time, it is desirable that talc is contained in an amount of 7 to 50 parts by weight based on 100 parts by weight of the total amount of the polymer component and talc.

Further, in the above resin composition, the interfacial strength of the flat interface between the component (B) and the ethylene-butene rubber has a phase angle of −2 ° to −12 according to the asymmetric double cantilever beam method. When measured in the ° range,
It is preferably 100 to 400 (J / m ² ).

In the first invention, the component (B) and the polyethylene-ethylene / propylene-
The interfacial strength of the flat interface between polyethylene triblock copolymers is asymmetric double cantilever beam method,
When the phase angle is measured in the range of −2 ° to −12 °,
It is preferably 100 to 1000 (J / m ² ).

In the second aspect, the component (B) and the polystyrene-ethylene / propylene-
The interfacial strength of the flat interface between polyethylene triblock copolymers is asymmetric double cantilever beam method,
When the phase angle is measured in the range of −2 ° to −12 °,
It is preferably 100 to 1000 (J / m ² ).

Further, the interfacial strength of the flat interface between the component (A) which is soluble in 90 ° C. xylene of the polypropylene polymer and the component (B) has a phase angle determined by the asymmetric double cantilever beam method. It is more preferably 50 to 400 (J / m ² ) when measured in the range of −2 ° to −12 °.

Further, in the above resin composition, the interfacial strength of the flat interface between the component (B) and the ethylene-butene rubber is from -2 ° to-° by the asymmetric double cantilever beam method. When measured in the range of 12 °, it is preferably 150 to 400 (J / m ² ).

Further, in the first invention, the component (B) and the polyethylene-ethylene / propylene-
The interfacial strength of the flat interface between the polyethylene triblock copolymers is 2 when the phase angle is measured by the asymmetric double cantilever beam method in the range of −2 ° to −12 °.
More preferably, it is from 0 to 1000 (J / m ² ).

Further, in the second invention, the component (B) and the polystyrene-ethylene / propylene-
The interfacial strength of the flat interface between the polyethylene triblock copolymers is 2 when the phase angle is measured by the asymmetric double cantilever beam method in the range of −2 ° to −12 °.
It is desirable that it is from 00 to 1000 (J / m ² ).

In the present invention, the polymer component 9
It is more preferable that the 0 ° C xylene-soluble component is 5% by weight or less in the total molecular weight of 2500 or less in terms of PP in the molecular weight measurement method by GPC in 140 ° C o-dichlorobenzene.

When talc is contained,
More preferably, the average particle size of the talc is 2.5 μm or less. Hereinafter, the present invention will be described in detail.

[Polypropylene-based Polymer] The polypropylene-based polymer in the present invention is required to contain at least a propylene-ethylene block copolymer in its components. That is, the polypropylene-based polymer in the present invention may be the propylene-ethylene block copolymer alone.
In addition to ethylene block copolymer, random copolymer or propylene homopolymer (homopolypropylene)
Can also be used in combination. As the comonomer of the random copolymer, α-olefins other than propylene such as ethylene, butene-1, pentene-1, and hexene-1 are used, and among them, ethylene is particularly preferable. In the block copolymer using ethylene as the α-olefin, the ethylene-propylene block in the molecule is dispersed in the homopolypropylene block and exhibits rubber elasticity, and functions as a rubber component. The polypropylene polymer has a melt flow rate (according to JIS K6758; hereinafter referred to as MFR) of 5 to 100 g / 1.
0 minutes is preferred. If the MFR is less than 5 g / 10 minutes, the fluidity of the resin composition obtained will be poor, and the moldability will be impaired.
When R exceeds 100 g / 10 minutes, the impact resistance of the resin composition is poor. These polypropylene-based polymers may be those having a low MFR within the above range by kneading and bisbreaking with an organic peroxide.

The PP polymer having at least the propylene-ethylene block copolymer has a component (A) soluble in xylene at 90 ° C. and a component (B) insoluble in xylene at 110 ° C.
The interfacial strength of a flat interface between and (hereinafter referred to as Gc:
Defined by the critical strain energy release rate) by the asymmetric double cantilever beam method, the phase angle is from -2 ° to -12
When measured in the range of °, it is indispensable to be ^{20 to} 500 (J / m ² ). This value is 50-400
More preferably (J / m ² ). This is Gc is 2
If it is less than 0 (J / m ² ), the impact resistance of the resin composition obtained will decrease, and if Gc exceeds 500 (J / m ² ), the resistance of the resin composition obtained in the same manner as above will be low. This is because the impact resistance is reduced.

[Ethylene-Butene Rubber] The Gc of the flat interface between the ethylene-butene rubber used in the present invention and the above-mentioned component (B) has a phase angle of −2 ° by the asymmetric double cantilever beam method. It is preferably 100 to 400 (J / m ² ) when measured in the range of from -12 °. Furthermore, this value is 150-400
More preferably (J / m ² ). This Gc is 100
When it is less than (J / m ² ) or more than 400 (J / m ² ), the impact resistance of the obtained resin composition is lowered.

[Polyethylene-ethylene / propylene-
Polyethylene triblock copolymer] In the first invention of the present invention, a polyethylene-ethylene / propylene-polyethylene triblock copolymer is further essential. The polyethylene-ethylene / propylene-polyethylene triblock copolymer has an ethylene / propylene copolymer block located at the center of the molecule and polyethylene blocks located on both sides thereof. Generally, it can be produced by hydrogenating an alternating copolymer of butadiene and isoprene. The interfacial strength of the flat interface between the polyethylene-ethylene / propylene-polyethylene triblock copolymer and the above-mentioned component (B) has a phase angle of − in the asymmetric double cantilever beam method.
100 to 10 when measured in the range of 2 ° to -12 °
It is preferably 00 (J / m ² ). 200-10
More preferably, it is 00 J / m ² . Interface strength is 100
J larger than / m ² or less than 1000 J / m ^2, the impact resistance of the resin composition obtained is lowered.

[Polystyrene-ethylene / propylene-
Polyethylene triblock copolymer] In the second invention of the present invention, a polystyrene-ethylene / propylene-polyethylene triblock copolymer is essential. In the polystyrene-ethylene / propylene-polyethylene triblock copolymer, an ethylene / propylene copolymer block is located at the center of the molecule, and polyethylene blocks and polystyrene blocks are located on both sides of the ethylene / propylene copolymer block. Generally, it can be produced by hydrogenating a styrene-butadiene polymer. The interfacial strength of the flat interface between this polyethylene-ethylene / propylene-polyethylene triblock copolymer and the above-mentioned component (B) has a phase angle of −2 ° to −12 ° by the asymmetric double cantilever beam method. When measured in the range of
It is preferably 100 to 1000 (J / m ² ).
It is more preferably 200 to 1000 J / m ² . And interface strength is greater than 100 J / m ² or less than 1000 J / m ^2, the impact resistance of the resulting resin composition is lowered.

[Talc] The talc used in the present invention preferably has an average particle size of 2.5 μm or less. This is because if the average particle size is larger than 2.5 μm, the elastic modulus, impact strength, and tensile strength tend to decrease.

[Composition Ratio] In the polymer component of the first invention, the ratio of the component soluble in xylene at 70 ° C. in the fractionation with xylene is 25 to 60 parts by weight with respect to the polymer component. This is because if the amount is less than 25 parts by weight, the impact resistance of the obtained resin composition is lowered, and if it exceeds 60 parts by weight, the rigidity is lowered.

Similarly, in the second invention, the proportion of the component soluble in xylene at 70 ° C. in the fractionation with xylene is 25 to 60 parts by weight with respect to the polymer component. 25
This is because if it is less than 60 parts by weight, the impact resistance of the obtained resin composition is lowered, and if it exceeds 60 parts by weight, the rigidity is lowered.

The resin composition of the present invention may contain talc. The content of talc is 7 to 50 per 100 parts by weight of the total amount of talc and the polymer component.
It is preferably part by weight. If the content of talc is less than 7 parts by weight, the rigidity and heat distortion resistance of the obtained resin composition will decrease, and if it exceeds 50 parts by weight, the impact resistance will decrease. The content of this talc is 8 to 45
More preferably, it is 10 parts by weight, and more preferably 10 to 40 parts by weight.

[Method of Measuring Interface Strength] In the present invention, the interface strength (Gc) is defined by the critical strain energy release rate of cracks existing at the interface. The asymmetric double cantilever beam method (hereinafter ADCB) is used to measure the Gc at the interface.
And ) Is used. This is because the cracks run along the interface. In the conventional peel test, it is not possible to grow cracks along the interface,
Gc at the interface cannot be measured accurately. The parameter that determines the crack growth direction is the phase angle ψ defined by the following equation. ψ = tan ⁻¹ (K _II / K _I ) where K _I and K _II are stress intensity factors for mode I and mode II. The phase angle ψ depends on the geometry of the ADCB, the elastic modulus of each material, the Poisson's ratio, and the crack length, but is numerically evaluated by the boundary element method (BEM) and the finite element method (FEM). In the present invention, it is necessary to measure Gc in a phase angle range of −2 ° to −12 °. When the crack propagates toward the thin beam, ψ
Is defined as negative. If the phase angle is less than -12 °, cracks at the interface will penetrate into the thinner material, and Gc
Can not be evaluated. On the other hand, when the phase angle is larger than −2 °, the growth of cracks at the interface is unstable, and similarly, Gc cannot be evaluated accurately.

Further, in the resin composition of the present invention, the 90 ° C. xylene soluble component of the polymer component is converted into PP in a molecular weight measurement method by GPC (gel permeation chromatography) in 140 ° C. o-dichlorobenzene. The total amount of components having a molecular weight of 2500 or less is preferably 5% by weight or less. It is more preferably 4% by weight or less, and further preferably 3% by weight or less. If this value is within the range of the present invention, the adhesive strength and heat resistance can be improved.

In producing the propylene-based resin composition of the present invention, heat, oxygen and light stabilizers, flame retardants, fillers, colorants, lubricants, plasticizers widely used in the field of synthetic resins and synthetic rubbers. Depending on the purpose of use, additives such as agents and antistatic agents may be added within a range that does not essentially impair the characteristics of the polypropylene resin composition of the present invention.

Examples of the antioxidant include the following. Dibutyl hydroxytoluene, alkylated phenol, 4,4'-thiobis- (6-t-butyl-3-methylphenol), 4,4'-butylidenebis- (6-t-butyl-3-methylphenol), 2, 2'-methylenebis- (4-methyl-6
-t-butylphenol), 2,2'-methylenebis- (4-methyl-6-t-butylphenol), 2,2'-methylenebis-
(4-Ethyl-6-t-butylphenol), 2,6-di-t-butyl-4-ethylphenol, 1,1,3-tris (2-methyl-4-hydroxy-5-t-butylphenyl) Butane, n-
Octadecyl-3- (4-hydroxy-3,5-di-t-butylphenyl) propionate, tetrakis [methylene-3-
(3,5-di-t-butyl-4-hydroxyphenyl) propionate] methane, dilaurylthiodipropionate,
Distearyl thiodipropionate, dimyristyl thiopropionate. Further, as the hindered phenol type, triethylene glycol-bis [3- (3-t-
Butyl-5-methyl-4-hydroxyphenyl) propionate], 1,6-hexanediol-bis [3- (3,5-di-
t-butyl-4-hydroxyphenyl) propionate],
2,4-bis- (n-octylthio) -6- (4-hydroxy-3,
5-di-t-butylanilino) -1,3,5-triazine, pentaerythrityl-tetrakis [3- (3,5-di-t-butyl-
4-hydroxyphenyl) propionate], 2,2-thio
-Diethylenebis [3- (3,5-di-t-butyl-4-hydroxyphenyl) propionate], octadecyl-3-
(3,5-di-t-butyl-4-hydroxyphenyl) propionate, N, N'-hexamethylenebis (3,5-di-t-butyl-4-hydroxy-hydrocinnamamide), 3.5 -The-t-
Butyl-4-hydroxy-benzylphosphonate-diethyl ester, 1,3,5-trimethyl-2,4,6-tris
(3,5-di-t-butyl-4-hydroxybenzyl) benzene, tris- (3,5, -di-t-butyl-4-hydroxybenzyl) -isocyanurate, octylated diphenylamine, 2,4- There is bis [(octylthio) methyl] -O-cresol. Examples of the hydrazine type include N, N'-bis [3- (3,5-di-t-butyl-4-hydroxyphenyl) propionyl] hydrazine. Besides, a phenol-based antioxidant, a phosphite-based antioxidant, a thioether-based antioxidant, a heavy metal deactivator, etc. can be applied.

Examples of the ultraviolet absorber include 2 (2'-
Hydroxy-5'-methylphenyl) benzotriazole,
2 (2'-hydroxy-3'-t-butyl-5'-methylphenyl) 5chlorobenzotriazole, 2 (2'-hydroxy-
3 ', 5-di-t-butylphenyl) 5chlorobenzotriazole, 2-hydroxy-4-n-octoxybenzophenone, phenyl salicylate, 2- (5-methyl-2-hydroxyphenyl) benzotriazole, 2- [ 2-hydroxy-
3,5-bis (α, α-dimethylbenzyl) phenyl] -2H-
Benzotriazole, 2- (3,5-di-t-butyl-2-hydroxyphenyl) benzotriazole, 2- (3-t-butyl-5-methyl-2-hydroxyphenyl) -5-chlorobenzotriazole, 2 -(3,5-di-t-butyl-2-hydroxyphenyl) -5-chlorobenzotriazole, 2- (3,5
-Di-t-amyl-2-hydroxyphenyl) benzotriazole, 2- (2'-hydroxy-5'-t-octylphenyl)
Examples include benzotriazole and hydroxyphenyl benzotriazole derivatives. Or dimethyl succinate
1- (2-hydroxyethyl) -4-hydroxy-2,2,6,6
-Tetramethylpiperidine polycondensate, poly [{6- (1,
1,3,3-Tetramethylbutyl) amino-1,3,5-triazine-2,4-diyl} {(2,2,6,6-tetramethyl-4-
Hyperidyl) imino} hexamethylene {(2,2,6,6-tetramethyl-4-piperidyl) imino}], N, N'-bis
(3-Aminopropyl) ethylenediamine ・ 2,4-bis [N-butyl-N- (1,2,2,6,6-pentamethyl-4piperidyl) amino] -6-chloro-1,3,5-triazine Condensate, bis (2,2,6,6-tetramethyl-4-piperidyl) sebacate, 2- (3,5-di-t-butyl-4-hydroxybenzyl) -2-n-butylmalonate bis ( 1,2,2,6,6-pentamethyl-4-piperidyl), 2,4-di-t-butylphenyl-3,5-di-t-butyl-4-hydroxybenzoate and the like.

As the flame retardant, for example, the following can be applied. Polybromodiphenyl oxide, tetrabromobisphenol A, brominated epoxyhexabromocyclododecane, ethylenebistetrabrimophthalimide, brominated polystyrene dechlorane, brominated polycarbonate, polyphosphonate compound, halogenated polyphosphonate, triazine, red phosphorus, Tricresyl phosphate, triphenyl phosphate, cresyl diphenyl phosphate, triallyl phosphate, trixylyl phosphate, trialkyl phosphate, trischloroethyl phosphate, trischloropropyl phosphate, tris (dichloropropyl phosphate), antimony trioxide, aluminum hydroxide, Magnesium hydroxide. Or silicone oil, stearic acid, calcium stearate, carbon black, titanium dioxide,
Silica, mica, montmorillonite, etc.

[Production Method of Resin Composition] The propylene resin composition of the present invention is produced by uniformly mixing the above-mentioned components and additives. The compounding method (mixing method) is not particularly limited, and a method generally used in the field of synthetic resins may be applied. As a mixing method, generally used is a method of dry blending using a mixer such as a Henschel mixer, a tumbler and a ribbon mixer, and a melting method such as an open roll, an extrusion mixer, a kneader and a Banbury mixer. The method of mixing is mentioned. Among these methods, in order to obtain a more uniform resin composition, it is advisable to use two or more of these mixing methods in combination. For example, after dry blending in advance, the mixture is melt mixed. In the case of using dry blending together, even in the case of using one or two or more methods of melt mixing, it is particularly preferable to produce pellets by using a pelletizer when producing a molded article by the molding method described below. . Among the above mixing methods, it is necessary to carry out at a temperature at which the resin used is melted, regardless of whether the resin is melt-mixed or molded by the molding method described later. However, if it is carried out at a high temperature, the resin will be thermally decomposed and deteriorated.
It is carried out at 350 ° C. (preferably 190 to 260 ° C.).

The resin composition of the present invention can be molded into a desired shape by applying a molding method such as an injection molding method, an extrusion molding method, a compression molding method and a hollow molding method which are generally used in the field of synthetic resins. Good. Alternatively, after being formed into a sheet using an extrusion molding machine, this sheet may be formed into a desired shape by a secondary processing method such as a vacuum forming method or a pressure forming method.

[0034]

【Example】

[First Example] Various propylene-ethylene copolymers of high impact polypropylene (HIPP) shown in Table 1 and ethylene-butene rubber (EBR)
, Polyethylene-ethylene / propylene-polyethylene triblock copolymer (TBC) and talc were mixed in the proportions shown in Table 2, and dry blended for 5 minutes with a Henschel mixer. The obtained mixture was kneaded using the same-direction twin-screw extruder (diameter 30 mm) set at 210 ° C. to produce pellets made of the resin compositions having the compositions of Examples 1-8 and Comparative Examples 1-7. . For example, the resin composition of Example 1 shown in Table 2 is the polypropylene polymer (PP-1) shown in Table 1, ethylene-butene rubber (EBR-1), and triblock. Copolymer (TBC
-1) and talc (talc 1), 70: 7: 13:
It was mixed at a compounding ratio of 10. The obtained pellets of each resin composition were injection-molded using an injection molding machine set at 230 ° C. to prepare a test piece for measurement.
The proportion of components soluble in xylene, flexural modulus, Izod impact strength, heat distortion temperature, and tensile property were measured. The measurement results are shown in Table 2.

In the table, the strength of the planar interface between the component (A) and the component (B) is Gc (A / B), and the strength of the planar interface between the EBR and the component (B) is Gc ( EBR / B),
The strength of the planar interface between TBC and the component (B) is Gc (T
BC / B). The particle size of talc was determined by using the light scattering sedimentation method, and the central particle size was determined to be the particle size of talc. Also,
The FB column shows the propylene weight fraction (% by weight) in EBR, and FE shows the ethylene content of the triblock copolymer, which was measured by NMR. Moreover, various physical properties in Table 2 were measured as follows. Flexural modulus (kgf / cm ² ) is ASTM D
According to 790, it was measured at a temperature of 23 ° C.

Izod impact strength (IZOD: kgf · cm / c
m) was measured with a notch according to ASTM D265 at a temperature of -30 ° C. Heat distortion temperature (HDT) is A
It was measured according to STM D648 under a load of 66 psi. Tensile properties were measured according to ASTM D638 at a temperature of 23 ° C.

The interfacial strength Gc is calculated as "closed loop (Cl
osed Loop) ", 1990, Vol. 23, p. 3929. That is, first, two flat plates made of the component (B) having different thicknesses are press-molded and prepared.
Further, a film having a thickness of 10 μm, which comprises the component (A) or EBR to be tested, is produced. Then, as shown in FIG. 1, the flat plates of the component (B) were superposed so as to sandwich the film of the component (A) or the EBR, held at 180 ° C. under a load of 3 kg for 10 minutes, and adhered to each other, and then tested for Gc measurement. Let's just cut it. Then, insert a wedge between the interfaces and let it stand at room temperature for 24 hours.
After leaving for a while, the crack length generated at the tip of the wedge was measured to calculate the interface strength Gc. The thickness ratio of the flat plate was controlled so that the phase angle was −7 °. The phase angle is
It was calculated by the BEM method (boundary element method).

[0038]

[Table 1]

[0039]

[Table 2]

From the results shown in Table 2, it is clear that all the resin compositions of Examples 1 to 8 have high flexural modulus and Izod impact strength, high heat resistance and high extensibility. is there. However, the interface strength Gc (EB
In the case of Comparative Example 1 in which EBR having a small R / B) of 60 is used, the impact resistance is small. Further, the interface strength Gc (EBR / B) is as large as 630, and the EB
Also in Comparative Example 2 in which R is used, the impact resistance is small. Furthermore, in Comparative Example 3 in which HIPP having a small interface strength Gc (A / B) of 15 is used,
The impact resistance has decreased.

In Comparative Example 4 in which talc having a large particle size of 5.6 μm was used, the impact resistance was small. In Comparative Example 5 in which xylene dissolution was as large as 70 parts by weight, the flexural modulus was low and the heat resistance was low. The comparative example 6 using TBC having a small interface strength Gc (TBC / B) of 50 has a low impact resistance. T
In Comparative Example 7 having no BC, not only the impact resistance is small, but also the elongation is small.

[Second Embodiment] Similarly, various polypropylene polymers (HIPP), ethylene-butene rubber (EBR), and polystyrene-ethylene / propylene-polyethylene triblock copolymers shown in Table 3 are similarly prepared. (T
BC) and talc were blended in the proportions shown in Table 4, and dry blended for 5 minutes with a Henschel mixer. The obtained mixture was kneaded using a co-direction twin-screw extruder (diameter 30 mm) set to 210 ° C. to produce pellets composed of the resin compositions of Examples 9 to 15 and Comparative Examples 8 to 14. . For example, the resin composition of Example 9 shown in Table 4 contains the polypropylene polymer (PP-1) shown in Table 3 and the ethylene-butene rubber (EBR-).
5), the triblock copolymer (TBC-4), and talc (talc 1) were mixed at a compounding ratio of 70: 7: 13: 10. The obtained pellets of each resin composition were injection-molded using an injection molding machine set at 230 ° C. to prepare a test piece for measurement, which was converted into 90 ° C. xylene in the same manner as in the first example. The proportion of soluble components, flexural modulus, Izod impact strength, heat distortion temperature and tensile strength were measured. The measurement results are shown in Table 2.

In the table, the strength of the planar interface between the component (A) and the component (B) is Gc (A / B), and the strength of the planar interface between the EBR and the component (B) is Gc ( EBR / B),
The strength of the planar interface between TBC and the component (B) is Gc (T
BC / B). The particle size of talc was determined by using the light scattering sedimentation method, and the central particle size was determined to be the particle size of talc. Also,
FB indicates the ethylene content in EBR, and NMR
It was measured in. FE represents the ethylene content of the triblock copolymer, which was measured by NMR. FS represents the styrene content of the triblock copolymer, which was measured by NMR.

[0044]

[Table 3]

[0045]

[Table 4]

From the results shown in Table 4, it is clear that all the resin compositions of Examples 9 to 15 have high flexural modulus and Izod impact strength, high heat resistance, and high extensibility. is there. However, the interface strength Gc (E
Comparative Example 8 using EBR having a small BR / B) of 50
In this case, the impact resistance is reduced. The impact resistance of Comparative Example 9 having a large interface strength Gc (EBR / B) of 630 is also low.

Further, in Comparative Example 10 using HIPP having a small interface strength Gc (A / B) of 15, the impact resistance is small. In Comparative Example 11 in which talc having a large particle size of 5.6 μm is used, the impact resistance is small. In Comparative Example 12 in which xylene dissolution was as large as 70 parts by weight, the bending elastic modulus was small,
And the heat resistance is low. Interfacial strength Gc (TBC / B) is 50
The comparative example 13 using a small TBC has a low impact resistance. Comparative Example 14 without TBC
Not only has low impact resistance, but also low elongation.

[0048]

The invention according to claim 1 of the present invention comprises a polypropylene polymer having at least a propylene-ethylene block copolymer in its component, an ethylene-butene rubber, and a polyethylene-ethylene / propylene-polyethylene. It has a polymer component containing a triblock copolymer and has a temperature of 70 ° C. when fractionated with xylene.
The proportion of the xylene-soluble component is 25 to 60 parts by weight, and it is between the component (A) soluble in 90 ° C xylene and the component (B) insoluble in 110 ° C xylene of the polypropylene polymer. The interface strength of the flat interface has a phase angle of −2 ° to −12 ° by the asymmetric double cantilever beam method.
It is 20-500 (J / m < ² >) when measured in the range of.

According to the second aspect of the invention, a polypropylene polymer having at least a propylene-ethylene block copolymer in its components, an ethylene-butene rubber, and a polystyrene-ethylene / propylene-polyethylene triblock copolymer. And a proportion of the component soluble in 70 ° C. xylene in the fractionation with xylene is 25 to 60 parts by weight, and the polypropylene polymer is soluble in 90 ° C. xylene. The interfacial strength of the flat interface between the component (A) and the component (B) insoluble in 110 ° C xylene was measured by the asymmetric double cantilever beam method in the phase angle range of -2 ° to -12 °. When it does, it is 20-500 (J / m < ² >), It is a resin composition characterized by the above-mentioned.

According to the invention of claim 3, the talc is 7 to 50.
The resin composition according to claim 1 or 2, wherein the resin composition is contained in an amount by weight.

The invention according to claim 4 is the same as claims 1, 2, and 3.
In the resin composition according to any one of items 1 to 5, the interface strength of the flat interface between the component (B) and the ethylene-butene rubber has an asymmetric double cantilever beam phase angle of −2 ° to −. The resin composition is 100 to 400 (J / m ² ) when measured in a range of 12 °.

According to a fifth aspect of the invention, in the resin composition according to the first aspect, the interfacial strength of a flat interface between the component (B) and the polyethylene-ethylene / propylene-polyethylene triblock copolymer. However, the asymmetric double cantilever beam method has a phase angle of −2 ° to −12 °
It is 100-1000 (J / m < ² >) when it measures in the range of.

According to a sixth aspect of the present invention, in the resin composition according to the second aspect, the interfacial strength of the flat interface between the component (B) and the polystyrene-ethylene / propylene-polyethylene triblock copolymer is high. However, the asymmetric double cantilever beam method has a phase angle of −2 ° to −12 °
It is 100-1000 (J / m < ² >) when it measures in the range of.

A seventh aspect of the present invention is the resin composition according to any one of the first to sixth aspects, wherein the polypropylene polymer has a component (A) soluble in 90 ° C. xylene and the component (B). ), The interfacial strength of the flat interface with the asymmetric double cantilever beam method changes the phase angle from -2 ° to-
It is a resin composition characterized in that it is 50 to 400 (J / m ² ) when measured in the range of 12 °. The invention according to claim 8 is the resin composition according to any one of claims 1 to 7, wherein the interface strength of the flat interface between the component (B) and the ethylene-butene rubber is asymmetric double. The resin composition has a phase angle of 150 to 400 (J / m ² ) when measured by the cantilever beam method in the range of −2 ° to −12 °.

The invention according to claim 9 is the invention according to claim 1 or 5.
In the resin composition according to item 1, the interface strength of the flat interface between the component (B) and the polyethylene-ethylene / propylene-polyethylene triblock copolymer has a phase angle determined by an asymmetric double cantilever beam method- 200 to 1000 when measured in the range of 2 ° to -12 °
(J / m ² ), which is a resin composition.

The invention according to claim 10 is the resin composition according to claim 2 or 6, wherein a flat interface between the component (B) and the polystyrene-ethylene / propylene-polyethylene triblock copolymer is provided. Interface strength of
Phase angle of -2 ° with asymmetric double cantilever beam method
From 200 to 100 when measured in the range of −12 °
The resin composition is 0 (J / m ² ).

The invention according to claim 11 is the resin composition according to claim 2, characterized in that the average particle size of talc is 2.5 μm or less.

According to the present invention, which has the above structure,
In addition to having excellent impact resistance and high rigidity, it also has excellent heat resistance and tensile strength. Therefore, it is particularly suitable as a material for automobile interior and exterior parts.

[Brief description of drawings]

FIG. 1 is a side view for explaining a method for measuring an interface strength Gc.

 ─────────────────────────────────────────────────── ─── Continuation of the front page (72) Inventor Ikuminori Jinagawa, Toyota Town, Toyota City, Aichi Prefecture, 1st Toyota Automobile Co., Ltd. (72) Inventor Takesumi Nishio 1 Toyota Town, Toyota City, Aichi Prefecture Toyota Motor Co., Ltd.

Claims (11)

[Claims] 1. A polymer containing a polypropylene polymer having at least a propylene-ethylene block copolymer as a component, an ethylene-butene rubber, and a polyethylene-ethylene / propylene-polyethylene triblock copolymer. In the fractionation with xylene, the proportion of the component soluble in 70 ° C. xylene is 25 to 60 parts by weight, and the component (A) soluble in 90 ° C. xylene of the polypropylene polymer is used. , 110 ° C. The interfacial strength of the flat interface with the insoluble component (B) in xylene is 20 to 20 when the phase angle is measured in the range of −2 ° to −12 ° by the asymmetric double cantilever beam method. A resin composition, which is 500 (J / m ² ). 2. A polymer containing a polypropylene polymer having at least a propylene-ethylene block copolymer as a component, an ethylene-butene rubber, and a polystyrene-ethylene / propylene-polyethylene triblock copolymer. In the fractionation with xylene, the proportion of the component soluble in 70 ° C. xylene is 25 to 60 parts by weight, and the component (A) soluble in 90 ° C. xylene of the polypropylene polymer is used. , 110 ° C. The interfacial strength of the flat interface with the insoluble component (B) in xylene is 20 to 20 when the phase angle is measured in the range of −2 ° to −12 ° by the asymmetric double cantilever beam method. A resin composition, which is 500 (J / m ² ). 3. The resin composition according to claim 1, wherein talc is contained in an amount of 7 to 50 parts by weight based on 100 parts by weight of the total amount of the polymer component and talc. 4. The resin composition according to claim 1, 2, or 3, wherein the component (B) and the ethylene-
The interfacial strength of the flat interface between butene-based rubbers varies from -2 ° to -1 by the asymmetric double cantilever beam method.
When measured in the range of 2 °, 100 to 400 (J / m
² ) A resin composition characterized in that 5. The resin composition according to claim 1, wherein the interface strength of the flat interface between the component (B) and the polyethylene-ethylene / propylene-polyethylene triblock copolymer is asymmetric double cantilever. A resin composition having a phase angle of 100 to 1000 (J / m ² ) when measured by a beam method in a range of −2 ° to −12 °. 6. The resin composition according to claim 2, wherein the interface strength of the flat interface between the component (B) and the polystyrene-ethylene / propylene-polyethylene triblock copolymer is asymmetric double cantilever. A resin composition having a phase angle of 100 to 1000 (J / m ² ) when measured by a beam method in a range of −2 ° to −12 °. 7. The resin composition according to any one of claims 1 to 6, wherein a flat surface between the component (A) soluble in 90 ° C. xylene and the component (B) of the polypropylene polymer. A resin composition having an interface strength of 50 to 400 (J / m ² ) when the phase angle is measured in the range of −2 ° to −12 ° by the asymmetric double cantilever beam method. Stuff. 8. The resin composition according to claim 1, wherein the interface strength of the flat interface between the component (B) and the ethylene-butene rubber is asymmetric double cantilever beam. Phase angle from -2 ° to -12 °
150-400 (J / m ² ) when measured in the range
And a resin composition. 9. The resin composition according to claim 1, wherein the interface strength of the flat interface between the component (B) and the polyethylene-ethylene / propylene-polyethylene triblock copolymer is asymmetric. A resin composition having a phase angle of 200 to 1000 (J / m ² ) when measured in a range of −2 ° to −12 ° by the double cantilever beam method. 10. The resin composition according to claim 2 or 6, wherein the interface strength of the flat interface between the component (B) and the polystyrene-ethylene / propylene-polyethylene triblock copolymer is asymmetric. A resin composition having a phase angle of 200 to 1000 (J / m ² ) when measured in a range of −2 ° to −12 ° by the double cantilever beam method. 11. The resin composition according to claim 3, wherein the average particle diameter of talc is 2.5 μm or less.