WO2019117185A1 - Propylene-based resin composition and article molded from same - Google Patents

Propylene-based resin composition and article molded from same Download PDF

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Publication number
WO2019117185A1
WO2019117185A1 PCT/JP2018/045620 JP2018045620W WO2019117185A1 WO 2019117185 A1 WO2019117185 A1 WO 2019117185A1 JP 2018045620 W JP2018045620 W JP 2018045620W WO 2019117185 A1 WO2019117185 A1 WO 2019117185A1
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polypropylene resin
mass
parts
resin composition
surfactant
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PCT/JP2018/045620
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French (fr)
Japanese (ja)
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聡志 串
周一 高橋
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株式会社プライムポリマー
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Priority to JP2019559684A priority Critical patent/JPWO2019117185A1/en
Publication of WO2019117185A1 publication Critical patent/WO2019117185A1/en

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    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/01—Use of inorganic substances as compounding ingredients characterized by their specific function
    • C08K3/013—Fillers, pigments or reinforcing additives
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K5/00—Use of organic ingredients
    • C08K5/04—Oxygen-containing compounds
    • C08K5/10—Esters; Ether-esters
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K5/00—Use of organic ingredients
    • C08K5/16—Nitrogen-containing compounds
    • C08K5/20—Carboxylic acid amides
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
    • C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
    • C08L23/04—Homopolymers or copolymers of ethene
    • C08L23/08—Copolymers of ethene
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
    • C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
    • C08L23/10—Homopolymers or copolymers of propene

Definitions

  • the present invention relates to a polypropylene-based resin composition and a molded article thereof, and more particularly, to a polypropylene-based resin composition suitable for manufacturing automobile interior and exterior members such as pillar trims, door trims and door panels, and a molded article thereof.
  • Patent Document 1 a method of improving strength with a filler
  • Patent Document 2 a method of improving hardness by using a resin component excellent in crystallinity
  • Patent Document 3 a resin component excellent in crystallinity
  • Patent Document 3 Propylene resin composition excellent in protrusion whitening resistance and scratch resistance, containing a specific propylene / ethylene block copolymer, talc and fatty acid amide
  • Patent Document 5 a polypropylene resin composition which contains three types of specific polypropylene and a specific ethylene- ⁇ -olefin copolymer rubber and is excellent in physical property balance and scratch resistance
  • the present inventors can provide a resin composition in which the amount of bleeding of the lubricant and / or surfactant can be increased, even if the inorganic filler is not contained or the content of the inorganic filler is low, resistance to kicking. It was believed that scratch resistance would be improved and also surface properties other than kick and scratch resistance (eg abrasion resistance, scratch resistance) would also be improved. Moreover, since it was able to reduce content of an inorganic filler in connection with this, it considered that it was advantageous to weight reduction.
  • the object of the present invention is to provide a polypropylene resin composition which has a large amount of lubricant and / or surfactant bleed, is excellent in scratch resistance and other surface characteristics, and is capable of reducing the content of inorganic filler It is in providing a molded object.
  • the inventors of the present invention conducted intensive studies to solve the above problems, and as a result, the viscosity [(A) ⁇ ] of the polypropylene resin (A) and the viscosity of the ethylene / ⁇ -olefin copolymer (B) were measured under specific conditions. It is found that it is very effective to set the ratio of [(B) ⁇ ] [(B) ⁇ / (A) ⁇ ] within a specific low range and to make the blending amount of each component within a suitable range. , Completed the present invention. That is, the gist of the present invention is as follows.
  • the viscosity [(A)]] of the polypropylene resin (A) is 40 to 70 Pa ⁇ s
  • the viscosity [(B)]] of the ethylene / ⁇ -olefin copolymer (B) is 50 measured by the following method.
  • a polypropylene resin composition which has a ratio of (B) // (A)] of not more than 7.2 and not more than 330 Pa ⁇ s.
  • [Method of measuring viscosity] Viscosity of polypropylene resin (A) and ethylene / ⁇ -olefin copolymer (B) when flowing out from the capillary at a temperature of 210 ° C. and a shear rate of 1000 / s in a capillary having a length of 40 mm and an inner diameter of 1 mm.
  • the injection-molded article is washed with 10 mL of a dichloromethane washing solution and washed 10 mL of the washing solution was recovered and concentrated to 5 mL, and the test solution was subjected to gas chromatography, and the amount of the lubricant (D) bled on the surface of the injection molded body by the absolute calibration method. The amount of bleeding) and the amount of bleeding of the surfactant (E) which has been bled on the surface of the injection-molded product are determined.
  • the molded object which consists of a polypropylene resin composition as described in [6] [1].
  • the polypropylene resin composition of the present invention has a viscosity ratio measured under specific conditions of the polypropylene resin (A) and the ethylene / ⁇ -olefin copolymer (B) as the rubber component [(B) // (A) Since the ⁇ ] is relatively small, the amount of bleeding of the lubricant (D) and / or the surfactant (E) is large, and the resistance to kicking and other surface properties are excellent. In addition, since the surface properties such as the resistance to kicking are excellent, the content of the inorganic filler can be reduced. As a result, it is also advantageous for weight reduction.
  • the type of the polypropylene-based resin (A) used in the present invention is not particularly limited, and may be a propylene homopolymer or a copolymer of propylene and another monomer.
  • propylene homopolymer includes not only homopolymers obtained by polymerizing propylene alone but also polymers obtained by copolymerizing propylene and a small amount of ⁇ -olefin (substantially homopolymer). is there.
  • the small amount of ⁇ -olefin is preferably at least one ⁇ -olefin selected from the group consisting of ethylene and ⁇ -olefins of 4 to 8 carbon atoms. In particular, ethylene is preferred.
  • the propylene content is preferably at least 98 mol% and at most 100 mol%, and the content of at least one ⁇ -olefin selected from the group consisting of ethylene and ⁇ -olefins of 4 to 8 carbon atoms is preferred Is 0 mol% or more and 2 mol% or less.
  • the melt flow rate (MFR, 230 ° C., 21.16 kg) of the propylene homopolymer measured by the method according to JIS K 7210 is usually 10 g / 10 min or more and 300 g / 10 min or less.
  • the upper limit value of the melt flow rate range is preferably 270 g / 10 minutes, more preferably 250 g / 10 minutes.
  • the method for producing the propylene homopolymer is not particularly limited.
  • propylene can be homopolymerized in the presence of a known catalyst for olefin polymerization, or, if necessary, propylene can be polymerized with a small amount of ⁇ -olefin to obtain a propylene homopolymer.
  • a known catalyst for olefin polymerization or, if necessary, propylene can be polymerized with a small amount of ⁇ -olefin to obtain a propylene homopolymer.
  • the olefin polymerization catalyst include titanium-based catalysts and metallocene-based catalysts. In particular, titanium-based catalysts are preferred.
  • the ⁇ -olefin is preferably at least one ⁇ selected from the group consisting of ethylene and an ⁇ -olefin having 4 to 8 carbon atoms.
  • -An olefin more preferably at least one ⁇ -olefin selected from the group consisting of ethylene, 1-butene, 1-hexene and 1-octene, particularly preferably ethylene.
  • the content of at least one ⁇ -olefin selected from the group consisting of ethylene and ⁇ -olefins of 4 to 8 carbon atoms is preferably 15 mol% or more and 49 mol% or less, more preferably 20 mol% or more and 45 mol% or less is there.
  • the propylene / ⁇ -olefin copolymer may be a block copolymer or a random copolymer. In particular, block copolymers are preferred.
  • the melt flow rate (MFR, 230 ° C., 21.16 N load) of the propylene / ⁇ -olefin copolymer measured by the method according to JIS K 7210 is usually 0.5 g / 10 min or more and 80 g / 10 min or less Preferably it is 9 g / 10 minutes or more and 75 g / 10 minutes or less.
  • the propylene homopolymer and the propylene / ⁇ -olefin copolymer may be mixed.
  • a block copolymer having a segment of a propylene homopolymer and a segment of a propylene / ⁇ -olefin copolymer may be used.
  • the proportion of propylene homopolymer is preferably 0 to 65% by mass, more preferably 1 to 65% by mass, and particularly preferably 5 to 65% by mass, based on 100% by mass of the polypropylene resin (A).
  • the proportion of the olefin copolymer is preferably 35 to 100% by mass, more preferably 35 to 99% by mass, and particularly preferably 35 to 95% by mass.
  • the ethylene / ⁇ -olefin copolymer (B) used in the present invention is a copolymer containing ethylene as a main component.
  • the ⁇ -olefin is preferably at least one ⁇ -olefin selected from the group consisting of ⁇ -olefins of 3 to 8 carbon atoms, and more preferably propylene, 1-butene, 1-hexene and 1-octene And at least one ⁇ -olefin selected from the group consisting of Among these, 1-butene and 1-octene are particularly preferable.
  • the ethylene content of the ethylene / ⁇ -olefin copolymer (B) is preferably 65 mol% or more and 90 mol% or less, more preferably 75 mol% or more and 85 mol% or less.
  • the melt flow rate (MFR, 230 ° C., 21.16 N load) of ethylene / ⁇ -olefin copolymer (B) measured by the method according to JIS K 7210 is usually 0.5 g / 10 min or more, 80 g / 10 min. It is preferably at most 9 g / 10 minutes and at most 60 g / 10 minutes.
  • the type of the inorganic filler (C) used in the present invention is not particularly limited, and known inorganic fillers can be used.
  • Specific examples of the inorganic filler (C) include talc, mica, calcium carbonate, barium sulfate, glass fiber, gypsum, magnesium carbonate, magnesium oxide, titanium oxide and iron oxide.
  • metal powder or metal fiber which consists of metals, such as zinc, copper, iron, aluminum, is also mentioned.
  • talc, mica, calcium carbonate, glass fiber and the like are preferable, and talc is more preferable.
  • the average particle size of talc is preferably 1 to 15 ⁇ m, more preferably 1 to 6 ⁇ m.
  • ⁇ Lubricant (D)> The type of the lubricant (D) used in the present invention is not particularly limited, and known lubricants can be used.
  • the fatty acid amide may be a saturated fatty acid amide or an unsaturated fatty acid amide.
  • the fatty acid amide is preferably one or more fatty acid amides selected from the group consisting of fatty acid amides having 8 to 25 carbon atoms and dimers thereof, more preferably fatty acid amides having 8 to 25 carbon atoms, and having carbon atoms Fatty acid amides of 15 to 25 are particularly preferred.
  • fatty acid amides include oleic acid amide, stearic acid amide, erucic acid amide, behenic acid amide, palmitic acid amide, myristic acid amide, lauric acid amide, caprylic acid amide, caproic acid amide, n-oleylpalmitamide , N-oleyl erucamide, and their dimers.
  • oleic acid amide, stearic acid amide, erucic acid amide, behenic acid amide, and dimers thereof are preferable.
  • the fatty acid amide may be used alone or in combination of two or more.
  • the type of surfactant (E) used in the present invention is not particularly limited, and known surfactants can be used.
  • a surfactant which exerts an action as an antistatic agent in the polypropylene resin composition is preferable.
  • ester type surfactant is mentioned as a representative example of surfactant (E).
  • the ester type surfactant a compound having one or more ester groups having 8 to 25 carbon atoms is preferable, and a compound having one or more ester groups having 15 to 25 carbon atoms is more preferable.
  • the number of ester groups in these compounds is preferably one or two.
  • Specific examples of the ester type surfactant include glycerin fatty acid ester, diglycerin fatty acid ester, sorbitan fatty acid ester, sucrose fatty acid ester, alkyl glucoside, polyvalent carboxylic acid ester. Among them, glycerin fatty acid ester and diglycerin fatty acid ester are preferable.
  • glycerin fatty acid ester ie, fatty acid monoglyceride
  • fatty acid monoglyceride include stearic acid monoglyceride, oleic acid monoglyceride, linolenic acid monoglyceride, lauric acid monoglyceride, palmitic acid monoglyceride, myristic acid monoglyceride, behenic acid monoglyceride and margaric acid monoglyceride.
  • stearic acid monoglyceride and oleic acid monoglyceride are preferable.
  • diglycerin fatty acid esters include stearic acid diglyceride, oleic acid diglyceride, linolenic acid diglyceride, lauric acid diglyceride, palmitic acid diglyceride, myristic acid diglyceride, behenic acid diglyceride, margaric acid diglyceride .
  • stearic acid diglyceride and oleic acid diglyceride are preferable.
  • heat stabilizers if necessary, heat stabilizers, weather stabilizers, light stabilizers, antioxidants, antioxidants, fatty acid metal salts, softeners, dispersants, colorants, pigments
  • Other additives such as UV absorbers and nucleating agents may be blended within the scope of the purpose of the present invention.
  • the order of mixing of the components to be blended is optional. Each component may be mixed simultaneously, or a multistage mixing method may be used in which some components are mixed and then other components are mixed.
  • the viscosity [(A)]] of the polypropylene resin (A) measured by the following method is 40 to 70 Pa ⁇ s, an ethylene ⁇ ⁇ -olefin copolymer (B The viscosity [(B)]] is 50 to 330 Pa ⁇ s, and their ratio [(B) // (A)]] is 7.2 or less.
  • [Method of measuring viscosity] Viscosity of polypropylene resin (A) and ethylene / ⁇ -olefin copolymer (B) when flowing out from the capillary at a temperature of 210 ° C. and a shear rate of 1000 / s in a capillary having a length of 40 mm and an inner diameter of 1 mm. Measure
  • the viscosity [(A)]] of the polypropylene resin (A) is 40 to 70 Pa ⁇ s, preferably 42 to 65 Pa ⁇ s, more preferably 45 to 55 Pa ⁇ s.
  • the viscosity [(B)]] of the ethylene / ⁇ -olefin copolymer (B) is 50 to 330 Pa ⁇ s, preferably 50 to 300 Pa ⁇ s, more preferably 50 to 250 Pa ⁇ s.
  • the viscosity [(B)]] is appropriately low, physical properties such as tensile elongation are improved.
  • the ratio of the viscosity [(A) A] of the polypropylene resin (A) to the viscosity [(B)]] of the ethylene / ⁇ -olefin copolymer (B) [(B) ⁇ / (A)]] is 7. It is 2 or less, preferably 6.8 or less, more preferably 6.4 or less.
  • the total bleed amount of the lubricant (D) and the surfactant (E) measured by the following method is preferably 600 ⁇ g or more.
  • Method of measuring the amount of bleed After heat-treating an injection-molded article of polypropylene resin composition (size: length 240 mm, width 80 mm, thickness 3 mm) at a temperature of 50 ° C.
  • the injection-molded article is washed with 10 mL of a dichloromethane washing solution and washed 10 mL of the washing solution was recovered and concentrated to 5 mL, and the test solution was subjected to gas chromatography, and the amount of the lubricant (D) bled on the surface of the injection molded body by the absolute calibration method. The amount of bleeding) and the amount of bleeding of the surfactant (E) which has been bled on the surface of the injection-molded product are determined.
  • the bleed amount of the lubricant (D) is preferably 280 ⁇ g or more, more preferably 320 ⁇ g or more, particularly preferably 360 ⁇ g or more, and most preferably 450 ⁇ g or more.
  • the bleeding amount of the surfactant (E) is preferably 320 ⁇ g or more, more preferably 600 ⁇ g or more, particularly preferably 650 ⁇ g or more, and most preferably 700 ⁇ g or more.
  • the total bleed amount of the lubricant (D) and the surfactant (E) is preferably 600 ⁇ g or more, more preferably 800 ⁇ g or more, and particularly preferably 900 ⁇ g or more.
  • the amount of each component contained in the polypropylene resin composition of the present invention will be described.
  • the amount of each of these components is based on 100 parts by mass of components (A), (B) and (C) in total.
  • the amount of the polypropylene resin (A) is 49 to 90 parts by mass, preferably 50 to 90 parts by mass, and more preferably 70 to 90 parts by mass.
  • the amount of the ethylene / ⁇ -olefin copolymer (B) is 9 to 50 parts by mass, preferably 10 to 50 parts by mass, and more preferably 20 to 50 parts by mass.
  • the amount of the inorganic filler (C) is 0 parts by mass or more and less than 10 parts by mass. That is, the inorganic filler (C) may or may not be contained in the polypropylene resin composition of the present invention. When the inorganic filler (C) is contained, the amount is less than 10 parts by mass, preferably 0.1 parts by mass or more and less than 10 parts by mass, more preferably 0.2 to 8 parts by mass.
  • the polypropylene resin composition of the present invention contains both or one of a lubricant (D) and a surfactant (E).
  • lubricant (D) and surfactant (E) When both lubricant (D) and surfactant (E) are contained:
  • the amount of each of the lubricant (D) and the surfactant (E) is 0.2 to 0.6 parts by mass, preferably 0.3 to 0.5 parts by mass.
  • the amount of the lubricant (D) or surfactant (E) is more than 0.6 parts by mass and 1.2 parts by mass or less, preferably 0.7 to 1.0 parts by mass, more preferably 0.7 to It is 0.9 parts by mass.
  • a polypropylene resin composition can be obtained by mixing or melt-kneading each component with a mixing apparatus such as a Banbury mixer, a single screw extruder, a twin screw extruder, or a high speed twin screw extruder.
  • a mixing apparatus such as a Banbury mixer, a single screw extruder, a twin screw extruder, or a high speed twin screw extruder.
  • the polypropylene resin composition of the present invention is excellent in moldability, it can be used in various molding methods.
  • Specific examples of the molded article of the present invention include injection molded articles, foam molded articles, injection foam molded articles, extrusion molded articles, blow molded articles, vacuum / pressure molded articles, calendar molded articles, stretched films, and inflation films. .
  • injection molded articles are preferred.
  • the molding conditions in the case of manufacturing a molded object are not particularly limited, and known conditions can be adopted.
  • the molded article of the present invention has excellent moldability.
  • the polypropylene-based resin (A) since it is contained, it has sufficient rigidity, and since it contains ethylene / ⁇ -olefin (B), it has sufficient impact resistance.
  • the amount of bleeding of the lubricant (D) and / or the surfactant (E) is large, resistance to scratching and other problems even when the inorganic filler is not contained or the content of the inorganic filler is small. Surface properties are excellent.
  • the application of the molded article of the present invention is not particularly limited. Specific examples of suitable applications include door panels, pillar trims, door trims, door lower garnish, automobile interior and exterior members such as instrument panels, engine room peripheral parts, other automobile parts, home appliance parts, food containers, beverage containers, medical containers It can be mentioned. Among them, applications of automobile interior and exterior members are preferable, and applications of automobile door members and applications of pillar members are particularly preferable.
  • C ⁇ Inorganic filler (C)> “C-1”: Talc (manufactured by Asada Powder Co., Ltd., trade name JM-209, average particle size (laser diffraction) 4 to 5 ⁇ m)
  • E-1 stearic acid monoglyceride (manufactured by Kao Corporation, Electro Stripper (registered trademark) TS-5)
  • Examples 1a to 10a and Comparative Examples 1a to 10a Each component (parts by mass) shown in Tables 1 to 4 and, as other additives, 0.1 part by mass of a phenolic antioxidant (manufactured by BASF, trade name Irganox (registered trademark) 1010), phosphorus antioxidant Agent (BASF, trade name Irgafos 168) 0.05 parts by weight, hindered amine light stabilizer (ADEKA, trade name LA-52) 0.05 parts by weight, UV absorber (BASF, trade name Tinuvin (registered trademark)
  • a polypropylene resin composition was prepared containing 0.05 parts by mass of a trade mark 120) and 0.1 parts by mass of a nucleating agent (manufactured by ADEKA, trade name Adekastab (registered trademark) NA-11).
  • Component (A) is filled in a capillary with a length of 40 mm and an inner diameter of 1 mm using CAPIROGRAPH-1D manufactured by Toyo Seiki Seisakusho, and the component when flowing out from the capillary at a temperature of 210 ° C. and a shear rate of 1000 / s.
  • the viscosity [(A)]] of (A) was measured.
  • the viscosity [(B) ⁇ ] of the component (B) was also measured under the same conditions. And the ratio [(B) eta / (A) eta] of both was computed from these measured values.
  • a scuff kicking test device shown in FIG. 1 was used.
  • This scuff test device is equipped with a pedestal 3 for fixing a test piece 1 by a fixture (not shown), and a metal pendulum 7 and a pantograph 4 with a friction object (rubber test piece) 2 mounted on the tip. It is.
  • a friction material (rubber test piece) 2 a rubber piece having a Shore A surface hardness of 75 (manufactured by Hyundai Motor Co., Ltd., part number 18215-SA0-000) was used.
  • This device operates the pendulum 7 from the scratched test surface 6 of the test piece 1 from the height 5 of 20 cm, and the friction material (rubber test piece) 2 attached to the tip of the pendulum 7 is the test surface 6 of the test piece 1 By rubbing and passing through the top, it is possible to reproduce the state of kicking on the sole.
  • test was conducted according to the following operation procedure by two workers.
  • the test piece 1 was fixed on the pedestal 3 of the apparatus. 2.
  • the digital dip gauge was set on the upper part of the pendulum 7 and the tip of the gauge was placed on the upper part of the pendulum 7 to confirm that the scale of the gauge was 0 mm.
  • the lever of the pantograph 4 was rotated to raise the pedestal 3 so that the scale of the gauge was 0.3 mm. 4.
  • the tip of the pendulum 7 on which the rubber test piece 2 was mounted was pulled up to a height 5 of 20 cm from the scratched test surface 6. 5.
  • the pendulum 7 was released, and the rubber test piece 2 was rubbed against the test surface 6 of the test piece 1.
  • grade 5 is the best and grade 1 is the worst.
  • grade 1 The whitening of the surface of the friction part was remarkable remarkably.
  • 2 Whitening of the surface of the friction part was noticeable.
  • 3 The surface of the friction portion was slightly whitened.
  • 4" There was a trace that rubber rubbed on the friction part, but there was no whitening.
  • 5" There was neither a trace which rubber rubbed, nor whitening.
  • the polypropylene-based resin compositions of Comparative Examples 1a to 3a, 5a and 6a having relatively large ratios [(B) ⁇ / (A) ⁇ ] are bleeds of lubricant (D) and / or surfactant (E). The amount was low and the resistance to kicking was inferior.
  • the polypropylene resin composition of Comparative Example 4a not containing the rubber component ethylene / ⁇ -olefin copolymer (B) also has a low amount of bleeding of the lubricant (D) and / or the surfactant (E), Resistance to kicking was inferior.
  • the polypropylene resin compositions of Comparative Examples 7a to 10a having a large content of the inorganic filler (C) were improved in the resistance to kicking by the inorganic filler (C).
  • such a composition is not preferable from the viewpoint of weight reduction because the specific gravity of the composition as a whole is high.
  • Examples 1b to 12b and Comparative Examples 1 to 5b A polypropylene resin composition was prepared in the same manner as in Example 1a, except that the amounts of the respective components were changed as shown in Tables 5 to 7. The physical properties of these polypropylene resin compositions were measured or evaluated in the same manner as in Example 1a. The results are shown in Tables 5-7.
  • the polypropylene-based resin compositions of Comparative Examples 1b, 2b, 4b and 5b having relatively large ratios [(B) (/ (A) ⁇ ] are bleeds of the lubricant (D) and / or the surfactant (E). The amount was low and the resistance to kicking was inferior.
  • the polypropylene resin composition of Comparative Example 3b not containing the ethylene / ⁇ -olefin copolymer (B) which is a rubber component also has a low bleeding amount of the lubricant (D) and / or the surfactant (E). Resistance to kicking was inferior.
  • the polypropylene resin composition of the present invention is useful as a material for producing various molded articles such as injection molded articles.
  • the molded article of the present invention is very useful particularly as an automobile interior / exterior member such as a door panel, a pillar trim, a door trim, a door lower garnish, an instrument panel and the like.
  • Test piece 2 Friction material (rubber test piece) 3 pedestal 4 pantograph 5 height of pendulum (20 cm) 6 test surface 7 pendulum

Abstract

Disclosed is a polypropylene-based resin composition containing 49–90 parts by mass of a polypropylene-based resin (A), 9–50 parts by mass of an ethylene-alpha-olefin copolymer (B), and at least 0 parts by mass but less than 10 parts by mass of an inorganic filler (C), as well as (i) 0.2–0.6 parts by mass respectively of a lubricant (D) and a surfactant (E) or (ii) more than 0.6 parts by mass but no more than 1.2 parts by mass of a lubricant (D) or a surfactant (E) (wherein the total of components (A), (B), and (C) is 100 parts by mass); the viscosity [(A)η] of the polypropylene-based resin (A) being 40–70 Pa·s; the viscosity [(B)η] of the ethylene-alpha-olefin copolymer being 50–330 Pa·s; and the ratio [(B)η/(A)η) thereof being 7.2 or less.

Description

ポリプロピレン系樹脂組成物及びその成形体Polypropylene resin composition and molded article thereof
　本発明は、ポリプロピレン系樹脂組成物及びその成形体に関し、より詳しくは、ピラートリム、ドアトリム、ドアパネルなどの自動車内外装部材の製造に好適なポリプロピレン系樹脂組成物、及びその成形体に関する。 The present invention relates to a polypropylene-based resin composition and a molded article thereof, and more particularly, to a polypropylene-based resin composition suitable for manufacturing automobile interior and exterior members such as pillar trims, door trims and door panels, and a molded article thereof.
　ピラートリム、ドアトリム、ドアパネルなどの自動車内外装部材の原料としては、軽量で成形性に優れる各種樹脂の使用が試みられている。例えば、アクリロニトリル－スチレン系樹脂（ＡＳ系樹脂）又はポリプロピレン系樹脂（ＰＰ系樹脂）の表面をポリ塩化ビニル等の軟質樹脂表皮で被って皮革調に加飾した部材や、シボ加工したＡＳ系樹脂やＰＰ系樹脂表面に塗装を施して皮革調に加飾した部材が使用されている。 As materials for automobile interior and exterior members such as pillar trims, door trims, and door panels, use of various resins which are lightweight and excellent in formability has been attempted. For example, a member in which the surface of an acrylonitrile-styrene resin (AS resin) or a polypropylene resin (PP resin) is covered with a soft resin skin such as polyvinyl chloride and decorated in a leather-like manner, or an AS resin which is embossed And the member which painted on the PP system resin surface and was decorated in leather tone is used.
　近年、自動車の生産工程の簡略化や、使用後の材料のリサイクルの要求が高まって来ている。このような点から、自動車内外装部材においても、シボ加工などの表面加工を行った樹脂成形体を、塗装を施すことなく用いる要求が高まっている。しかし、塗装を施していないＰＰ系樹脂の成形体は、組み立て時や使用時に傷が生じ易い。 In recent years, demands for simplification of automobile production processes and recycling of used materials have been increasing. From this point of view, also in automobile interior and exterior members, there is an increasing demand to use a resin molded body which has been subjected to surface processing such as embossing and the like without coating. However, molded articles of PP resin not coated are easily damaged during assembly and use.
　そこで、自動車内外装部材として好適な特性を有すると共に、耐傷付き性に優れた成形体を製造する為の方法や組成物が提案されている。例えば、フィラーにより強度を向上させる方法（特許文献１参照）、結晶性に優れた樹脂成分を用いることにより硬度を向上させる方法（特許文献２参照）、タルク及び傷付き改良剤を含み、アイゾット衝撃強度及び耐傷付き性に優れるポリプロピレン系組成物（特許文献３参照）、特定のプロピレン・エチレンブロック共重合体とタルクと脂肪酸アミドを含み、耐突出白化性及び耐傷付き性に優れるプロピレン系樹脂組成物（特許文献４参照）、３種類の特定のポリプロピレンと特定のエチレン－α－オレフィン共重合体ゴムを含み、物性バランス及び耐傷付き性に優れるポリプロピレン系樹脂組成物（特許文献５参照）が提案されている。 Therefore, methods and compositions have been proposed for producing molded articles having properties suitable as automobile interior and exterior members and excellent in scratch resistance. For example, a method of improving strength with a filler (see Patent Document 1), a method of improving hardness by using a resin component excellent in crystallinity (see Patent Document 2), talc and a scratching improver, Izod impact Polypropylene composition excellent in strength and scratch resistance (see Patent Document 3), Propylene resin composition excellent in protrusion whitening resistance and scratch resistance, containing a specific propylene / ethylene block copolymer, talc and fatty acid amide (See Patent Document 4), a polypropylene resin composition (see Patent Document 5) which contains three types of specific polypropylene and a specific ethylene-α-olefin copolymer rubber and is excellent in physical property balance and scratch resistance is proposed. ing.
　さらに自動車内外装部材の用途においては、引っかき傷などの傷だけでなく、ゴム等の軟質物で擦ることによる表面状態の悪化もまた問題となる。自動車内外装部材の表面は、例えば靴底で蹴られる事態も生じ易いからである。そこで、２種類の特定のポリプロピレン系樹脂と特定のエチレン・α－オレフィン共重合体と脂肪酸アミド（滑剤）と界面活性剤を含み、耐足蹴り傷付き性に優れたポリプロピレン系樹脂組成物（特許文献６参照）が提案されている。 Furthermore, in the application of automobile interior and exterior members, not only scratches such as scratches, but also deterioration of the surface condition caused by rubbing with a soft material such as rubber becomes a problem. This is because the surface of the automobile interior and exterior member is likely to be kicked by, for example, the shoe sole. Therefore, a polypropylene resin composition which is excellent in resistance to kicking, comprising two specific polypropylene resins, a specific ethylene / α-olefin copolymer, a fatty acid amide (a lubricant) and a surfactant (patented patent) Reference 6) has been proposed.
特開２００９－０７９１１７号公報JP, 2009-079117, A 特開２０１２－１３２０２４号公報JP, 2012-132024, A 特開２００２－０６０５６０号公報JP, 2002-060560, A 特開２００３－０５５５２９号公報Japanese Patent Application Laid-Open No. 2003-055 529 特開２００４－０５１７６９号公報JP, 2004-051769, A 国際公開第２０１４／０４６０８６号International Publication No. 2014/046086
　本発明者らは、滑剤及び／又は界面活性剤のブリード量が多くなる樹脂組成物を提供できれば、無機充填剤を含まない又は無機充填剤の含有量が少ない場合であっても、耐足蹴り傷付き性が向上し、また耐足蹴り傷付き性以外の表面特性（例えば耐摩擦性、耐擦傷性）もまた向上するであろうと考えた。また、これに伴い無機充填剤の含有量を低減できるので、軽量化に有利であると考えた。 The present inventors can provide a resin composition in which the amount of bleeding of the lubricant and / or surfactant can be increased, even if the inorganic filler is not contained or the content of the inorganic filler is low, resistance to kicking. It was believed that scratch resistance would be improved and also surface properties other than kick and scratch resistance (eg abrasion resistance, scratch resistance) would also be improved. Moreover, since it was able to reduce content of an inorganic filler in connection with this, it considered that it was advantageous to weight reduction.
　すなわち本発明の目的は、滑剤及び／又は界面活性剤のブリード量が多く、耐足蹴り傷付き性及びその他の表面特性が優れ、無機充填剤の含有量を低減できるポリプロピレン系樹脂組成物及びその成形体を提供することにある。 That is, the object of the present invention is to provide a polypropylene resin composition which has a large amount of lubricant and / or surfactant bleed, is excellent in scratch resistance and other surface characteristics, and is capable of reducing the content of inorganic filler It is in providing a molded object.
　本発明者らは、上記課題を解決すべく鋭意検討した結果、特定条件で測定したポリプロピレン系樹脂（Ａ）の粘度［（Ａ）η］とエチレン・α－オレフィン共重合体（Ｂ）の粘度［（Ｂ）η］の比［（Ｂ）η／（Ａ）η］が特定の低い範囲内とし、且つ各成分の配合量を好適な範囲内とすることが非常に有効であることを見出し、本発明を完成した。すなわち、本発明の要旨は以下の通りである。 The inventors of the present invention conducted intensive studies to solve the above problems, and as a result, the viscosity [(A) η] of the polypropylene resin (A) and the viscosity of the ethylene / α-olefin copolymer (B) were measured under specific conditions. It is found that it is very effective to set the ratio of [(B) η] [(B) 比 / (A) η] within a specific low range and to make the blending amount of each component within a suitable range. , Completed the present invention. That is, the gist of the present invention is as follows.
［１］ポリプロピレン系樹脂（Ａ）４９～９０質量部、エチレン・α－オレフィン共重合体（Ｂ）９～５０質量部及び無機充填剤（Ｃ）０質量部以上１０質量部未満を含み、
　さらに、
（i）滑剤（Ｄ）及び界面活性剤（Ｅ）を各々０.２～０.６質量部、
若しくは、
（ii）滑剤（Ｄ）又は界面活性剤（Ｅ）を０.６質量部を超えて１.２質量部以下
含み、
［但し、成分（Ａ）、（Ｂ）及び（Ｃ）の合計を１００質量部とする。］
　以下の方法により測定される、ポリプロピレン系樹脂（Ａ）の粘度［（Ａ）η］が４０～７０Ｐａ・ｓ、エチレン・α－オレフィン共重合体（Ｂ）の粘度［（Ｂ）η］が５０～３３０Ｐａ・ｓであり、それらの比［（Ｂ）η／（Ａ）η］が７.２以下であるポリプロピレン系樹脂組成物。
　［粘度の測定方法］
　長さ４０ｍｍ、内径１ｍｍのキャピラリー内で、温度２１０℃、せん断速度１０００／ｓの条件で、キャピラリーから流出する際のポリプロピレン系樹脂（Ａ）及びエチレン・α－オレフィン共重合体（Ｂ）の粘度を測定する。 [1] 49 to 90 parts by mass of a polypropylene resin (A), 9 to 50 parts by mass of an ethylene / α-olefin copolymer (B), and 0 to 10 parts by mass of an inorganic filler (C),
further,
(I) 0.2 to 0.6 parts by mass of lubricant (D) and surfactant (E), respectively
Or
(Ii) more than 0.6 parts by mass and 1.2 parts by mass or less of a lubricant (D) or surfactant (E),
[However, the total of components (A), (B) and (C) is 100 parts by mass. ]
The viscosity [(A)]] of the polypropylene resin (A) is 40 to 70 Pa · s, and the viscosity [(B)]] of the ethylene / α-olefin copolymer (B) is 50 measured by the following method. A polypropylene resin composition which has a ratio of (B) // (A)] of not more than 7.2 and not more than 330 Pa · s.
[Method of measuring viscosity]
Viscosity of polypropylene resin (A) and ethylene / α-olefin copolymer (B) when flowing out from the capillary at a temperature of 210 ° C. and a shear rate of 1000 / s in a capillary having a length of 40 mm and an inner diameter of 1 mm. Measure
［２］以下の方法により測定される滑剤（Ｄ）及び界面活性剤（Ｅ）の合計ブリード量が６００μｇ以上である［１］に記載のポリプロピレン系樹脂組成物。
　［ブリード量の測定方法］
　ポリプロピレン系樹脂組成物の射出成形体（サイズ：縦２４０ｍｍ、横８０ｍｍ、厚さ３ｍｍ）を温度５０℃の条件で９時間熱処理した後、該射出成形体をジクロロメタン洗浄液１０ｍＬで洗浄し、洗浄後の該洗浄液１０ｍＬを回収して５ｍＬに濃縮したものを試験液とし、該試験液をガスクロマトグラフィーに供し、絶対検量線法により、射出成形体の表面にブリードしていた滑剤（Ｄ）の量（ブリード量）及び射出成形体の表面にブリードしていた界面活性剤（Ｅ）のブリード量を求める。 [2] The polypropylene resin composition according to [1], wherein the total bleed amount of the lubricant (D) and the surfactant (E) measured by the following method is 600 μg or more.
[Method of measuring the amount of bleed]
After heat-treating an injection-molded article of polypropylene resin composition (size: length 240 mm, width 80 mm, thickness 3 mm) at a temperature of 50 ° C. for 9 hours, the injection-molded article is washed with 10 mL of a dichloromethane washing solution and washed 10 mL of the washing solution was recovered and concentrated to 5 mL, and the test solution was subjected to gas chromatography, and the amount of the lubricant (D) bled on the surface of the injection molded body by the absolute calibration method. The amount of bleeding) and the amount of bleeding of the surfactant (E) which has been bled on the surface of the injection-molded product are determined.
［３］滑剤（Ｄ）が脂肪酸アミドである［１］に記載のポリプロピレン系樹脂組成物。 [3] The polypropylene resin composition according to [1], wherein the lubricant (D) is a fatty acid amide.
［４］脂肪酸アミドが、炭素原子数８～２５の脂肪酸アミド及びその２量体からなる群より選ばれる１種以上の脂肪酸アミドである［３］に記載のポリプロピレン系樹脂組成物。 [4] The polypropylene resin composition according to [3], wherein the fatty acid amide is at least one fatty acid amide selected from the group consisting of fatty acid amides having 8 to 25 carbon atoms and dimers thereof.
［５］界面活性剤（Ｅ）が、炭素原子数８～２５のエステル基を１つ以上有する化合物である［１］に記載のポリプロピレン系樹脂組成物。 [5] The polypropylene resin composition according to [1], wherein the surfactant (E) is a compound having one or more ester groups having 8 to 25 carbon atoms.
［６］［１］に記載のポリプロピレン系樹脂組成物からなる成形体。 The molded object which consists of a polypropylene resin composition as described in [6] [1].
［７］自動車内外装部材である［６］に記載の成形体。 [7] The molded article according to [6], which is an automobile interior and exterior member.
［８］自動車ドア部材又はピラー部材である［７］に記載の成形体。 [8] The molded article according to [7], which is a car door member or a pillar member.
　本発明のポリプロピレン系樹脂組成物は、ポリプロピレン系樹脂（Ａ）及びゴム成分であるエチレン・α－オレフィン共重合体（Ｂ）の特定条件で測定した粘度の比［（Ｂ）η／（Ａ）η］が比較的小さいので、滑剤（Ｄ）及び／又は界面活性剤（Ｅ）のブリード量が多く、耐足蹴り傷付き性及びその他の表面特性が優れている。また、耐足蹴り傷付き性などの表面特性が優れているので、無機充填剤の含有量を低減できる。その結果、軽量化にも有利である。 The polypropylene resin composition of the present invention has a viscosity ratio measured under specific conditions of the polypropylene resin (A) and the ethylene / α-olefin copolymer (B) as the rubber component [(B) // (A) Since the η] is relatively small, the amount of bleeding of the lubricant (D) and / or the surfactant (E) is large, and the resistance to kicking and other surface properties are excellent. In addition, since the surface properties such as the resistance to kicking are excellent, the content of the inorganic filler can be reduced. As a result, it is also advantageous for weight reduction.
　滑剤（Ｄ）及び／又は界面活性剤（Ｅ）のブリード量が多くなる理由は必ずしも明らかではない。ただし、おそらく両成分の粘度特性の差が小さいことによりゴム成分であるエチレン・α－オレフィン共重合体（Ｂ）が微分散し、これに伴いゴム成分間に存在するポリプロピレン系樹脂（Ａ）の領域が減少し、ゴム成分中に溶解拡散している滑剤（Ｄ）及び／又は界面活性剤（Ｅ）がゴム成分間を移行し易くなることに起因するものと考えられる。 The reason why the amount of bleeding of the lubricant (D) and / or the surfactant (E) is large is not always clear. However, probably because the difference between the viscosity characteristics of the two components is small, the ethylene / α-olefin copolymer (B) as the rubber component is finely dispersed, and along with this, the polypropylene resin (A) exists among the rubber components. It is considered that the area is reduced, and the lubricant (D) and / or the surfactant (E) dissolved and diffused in the rubber component is likely to move between the rubber components.
実施例におけるスカッフ足蹴り試験方法を説明する為の模式図である。It is a schematic diagram for demonstrating the scuff kicking test method in an Example.
　＜ポリプロピレン系樹脂（Ａ）＞
　本発明に用いるポリプロピレン系樹脂（Ａ）の種類は特に限定されず、プロピレン単独重合体であっても良いし、プロピレンと他のモノマーとの共重合体であっても良い。特に、少なくともプロピレン・α－オレフィン共重合体を含むことが好ましく、プロピレン・α－オレフィン共重合体及びプロピレン単独重合体を併せて含むことがより好ましい。 <Polypropylene resin (A)>
The type of the polypropylene-based resin (A) used in the present invention is not particularly limited, and may be a propylene homopolymer or a copolymer of propylene and another monomer. In particular, it is preferable to include at least a propylene / α-olefin copolymer, and it is more preferable to include a propylene / α-olefin copolymer and a propylene homopolymer together.
　プロピレン単独重合体とは、プロピレンのみを重合して得られるホモポリマーのみならず、プロピレンと少量のα－オレフィンを共重合して得られる重合体（実質的な単独重合体）を包含する意味である。この少量のα－オレフィンは、好ましくはエチレン及び炭素原子数４～８のα－オレフィンからなる群より選ばれる少なくとも１種のα－オレフィンである。特に、エチレンが好ましい。 The term "propylene homopolymer" includes not only homopolymers obtained by polymerizing propylene alone but also polymers obtained by copolymerizing propylene and a small amount of α-olefin (substantially homopolymer). is there. The small amount of α-olefin is preferably at least one α-olefin selected from the group consisting of ethylene and α-olefins of 4 to 8 carbon atoms. In particular, ethylene is preferred.
　プロピレン単独重合体において、プロピレン含量は好ましくは９８ｍｏｌ％以上、１００ｍｏｌ％以下であり、エチレン及び炭素原子数４～８のα－オレフィンからなる群より選ばれる少なくとも１種のα－オレフィンの含量は好ましくは０ｍｏｌ％以上、２ｍｏｌ％以下である。 In the propylene homopolymer, the propylene content is preferably at least 98 mol% and at most 100 mol%, and the content of at least one α-olefin selected from the group consisting of ethylene and α-olefins of 4 to 8 carbon atoms is preferred Is 0 mol% or more and 2 mol% or less.
　プロピレン単独重合体の、ＪＩＳ　Ｋ　７２１０に準拠した方法で測定したメルトフローレート（ＭＦＲ、２３０℃、２１.１６ｋｇ）は、通常１０ｇ／１０分以上、３００ｇ／１０分以下である。このメルトフローレートの範囲の上限値は、好ましくは２７０ｇ／１０分、より好ましくは２５０ｇ／１０分である。 The melt flow rate (MFR, 230 ° C., 21.16 kg) of the propylene homopolymer measured by the method according to JIS K 7210 is usually 10 g / 10 min or more and 300 g / 10 min or less. The upper limit value of the melt flow rate range is preferably 270 g / 10 minutes, more preferably 250 g / 10 minutes.
　プロピレン単独重合体の製造方法は特に限定されない。例えば、公知のオレフィン重合用触媒の存在下で、プロピレンを単独重合し、あるいは必要に応じてプロピレンを少量のα－オレフィンと共に重合してプロピレン単独重合体を得ることができる。オレフィン重合用触媒の具体例としては、チタン系触媒、メタロセン系触媒が挙げられる。特に、チタン系触媒が好ましい。 The method for producing the propylene homopolymer is not particularly limited. For example, propylene can be homopolymerized in the presence of a known catalyst for olefin polymerization, or, if necessary, propylene can be polymerized with a small amount of α-olefin to obtain a propylene homopolymer. Specific examples of the olefin polymerization catalyst include titanium-based catalysts and metallocene-based catalysts. In particular, titanium-based catalysts are preferred.
　ポリプロピレン系樹脂（Ａ）としてプロピレン・α－オレフィン共重合体を用いる場合、そのα－オレフィンは、好ましくはエチレン及び炭素原子数４～８のα－オレフィンからなる群より選ばれる少なくとも１種のα－オレフィンであり、より好ましくはエチレン、１－ブテン、１－へキセン及び１－オクテンがからなる群より選ばれる少なくとも１種のα－オレフィンであり、特に好ましくはエチレンである。エチレン及び炭素原子数４～８のα－オレフィンからなる群より選ばれる少なくとも１種のα－オレフィンの含量は、好ましくは１５ｍｏｌ％以上、４９ｍｏｌ％以下、より好ましくは２０ｍｏｌ％以上、４５ｍｏｌ％以下である。プロピレン・α－オレフィン共重合体は、ブロック共重合体でもあっても良いし、ランダム共重合体であっても良い。特に、ブロック共重合体が好ましい。 When a propylene-α-olefin copolymer is used as the polypropylene resin (A), the α-olefin is preferably at least one α selected from the group consisting of ethylene and an α-olefin having 4 to 8 carbon atoms. -An olefin, more preferably at least one α-olefin selected from the group consisting of ethylene, 1-butene, 1-hexene and 1-octene, particularly preferably ethylene. The content of at least one α-olefin selected from the group consisting of ethylene and α-olefins of 4 to 8 carbon atoms is preferably 15 mol% or more and 49 mol% or less, more preferably 20 mol% or more and 45 mol% or less is there. The propylene / α-olefin copolymer may be a block copolymer or a random copolymer. In particular, block copolymers are preferred.
　プロピレン・α－オレフィン共重合体のＪＩＳ　Ｋ　７２１０に準拠した方法で測定したメルトフローレート（ＭＦＲ、２３０℃、２１.１６Ｎ荷重）は、通常０.５ｇ／１０分以上、８０ｇ／１０分以下、好ましくは９ｇ／１０分以上、７５ｇ／１０分以下である。 The melt flow rate (MFR, 230 ° C., 21.16 N load) of the propylene / α-olefin copolymer measured by the method according to JIS K 7210 is usually 0.5 g / 10 min or more and 80 g / 10 min or less Preferably it is 9 g / 10 minutes or more and 75 g / 10 minutes or less.
　ポリプロピレン系樹脂（Ａ）が、プロピレン単独重合体及びプロピレン・α－オレフィン共重合体を用いる場合、プロピレン単独重合体とプロピレン・α－オレフィン共重合体を混合すれば良い。また、プロピレン単独重合体のセグメントと、プロピレン・α－オレフィン共重合体のセグメントを有するブロック共重合体を用いても良い。ポリプロピレン系樹脂（Ａ）１００質量％中、プロピレン単独重合体の割合は好ましくは０～６５質量％、より好ましくは１～６５質量％、特に好ましくは５～６５質量％であり、プロピレン・α－オレフィン共重合体の割合は好ましくは３５～１００質量％、より好ましくは３５～９９質量％、特に好ましくは３５～９５質量％である。 When the polypropylene-based resin (A) uses a propylene homopolymer and a propylene / α-olefin copolymer, the propylene homopolymer and the propylene / α-olefin copolymer may be mixed. Alternatively, a block copolymer having a segment of a propylene homopolymer and a segment of a propylene / α-olefin copolymer may be used. The proportion of propylene homopolymer is preferably 0 to 65% by mass, more preferably 1 to 65% by mass, and particularly preferably 5 to 65% by mass, based on 100% by mass of the polypropylene resin (A). The proportion of the olefin copolymer is preferably 35 to 100% by mass, more preferably 35 to 99% by mass, and particularly preferably 35 to 95% by mass.
　＜エチレン・α－オレフィン共重合体（Ｂ）＞
　本発明に用いるエチレン・α－オレフィン共重合体（Ｂ）は、エチレンを主成分とする共重合体である。α－オレフィンは、好ましくは炭素原子数３～８のα－オレフィンからなる群より選ばれる少なくとも１種のα－オレフィンであり、より好ましくはプロピレン、１－ブテン、１－へキセン及び１－オクテンからなる群より選ばれる少なくとも１種のα－オレフィンである。中でも、１－ブテン、１－オクテンが特に好ましい。 <Ethylene-α-olefin copolymer (B)>
The ethylene / α-olefin copolymer (B) used in the present invention is a copolymer containing ethylene as a main component. The α-olefin is preferably at least one α-olefin selected from the group consisting of α-olefins of 3 to 8 carbon atoms, and more preferably propylene, 1-butene, 1-hexene and 1-octene And at least one α-olefin selected from the group consisting of Among these, 1-butene and 1-octene are particularly preferable.
　エチレン・α－オレフィン共重合体（Ｂ）のエチレン含量は好ましくは６５ｍｏｌ％以上、９０ｍｏｌ％以下、より好ましくは７５ｍｏｌ％以上、８５ｍｏｌ％以下である。 The ethylene content of the ethylene / α-olefin copolymer (B) is preferably 65 mol% or more and 90 mol% or less, more preferably 75 mol% or more and 85 mol% or less.
　エチレン・α－オレフィン共重合体（Ｂ）のＪＩＳ　Ｋ　７２１０に準拠した方法で測定したメルトフローレート（ＭＦＲ、２３０℃、２１.１６Ｎ荷重）は、通常０.５ｇ／１０分以上、８０ｇ／１０分以下、好ましくは９ｇ／１０分以上、６０ｇ／１０分以下である。 The melt flow rate (MFR, 230 ° C., 21.16 N load) of ethylene / α-olefin copolymer (B) measured by the method according to JIS K 7210 is usually 0.5 g / 10 min or more, 80 g / 10 min. It is preferably at most 9 g / 10 minutes and at most 60 g / 10 minutes.
　＜無機充填剤（Ｃ）＞
　本発明に用いる無機充填剤（Ｃ）の種類は特に限定されず、公知の無機充填剤を使用できる。無機充填剤（Ｃ）の具体例としては、タルク、マイカ、炭酸カルシウム、硫酸バリウム、ガラス繊維、石膏、炭酸マグネシウム、酸化マグネシウム、酸化チタン、酸化鉄が挙げられる。さらに、亜鉛、銅、鉄、アルミニウム等の金属からなる金属粉末又は金属繊維も挙げられる。中でも、タルク、マイカ、炭酸カルシウム、ガラス繊維等が好ましく、タルクがより好ましい。タルクの平均粒径は、好ましくは１～１５μｍ、より好ましくは１～６μｍである。 <Inorganic filler (C)>
The type of the inorganic filler (C) used in the present invention is not particularly limited, and known inorganic fillers can be used. Specific examples of the inorganic filler (C) include talc, mica, calcium carbonate, barium sulfate, glass fiber, gypsum, magnesium carbonate, magnesium oxide, titanium oxide and iron oxide. Furthermore, metal powder or metal fiber which consists of metals, such as zinc, copper, iron, aluminum, is also mentioned. Among them, talc, mica, calcium carbonate, glass fiber and the like are preferable, and talc is more preferable. The average particle size of talc is preferably 1 to 15 μm, more preferably 1 to 6 μm.
　＜滑剤（Ｄ）＞
　本発明に用いる滑剤（Ｄ）の種類は特に限定されず、公知の滑剤を使用できる。滑剤（Ｄ）としては、脂肪酸アミド、金属石鹸、炭化水素が好ましく、脂肪酸アミドがより好ましい。 <Lubricant (D)>
The type of the lubricant (D) used in the present invention is not particularly limited, and known lubricants can be used. As the lubricant (D), fatty acid amides, metal soaps and hydrocarbons are preferable, and fatty acid amides are more preferable.
　脂肪酸アミドは、飽和脂肪酸アミドであっても良いし、不飽和脂肪酸アミドであっても良い。脂肪酸アミドとしては、炭素原子数８～２５の脂肪酸アミド及びその２量体からなる群より選ばれる１種以上の脂肪酸アミドが好ましく、炭素原子数８～２５の脂肪酸アミドがより好ましく、炭素原子数１５～２５の脂肪酸アミドが特に好ましい。 The fatty acid amide may be a saturated fatty acid amide or an unsaturated fatty acid amide. The fatty acid amide is preferably one or more fatty acid amides selected from the group consisting of fatty acid amides having 8 to 25 carbon atoms and dimers thereof, more preferably fatty acid amides having 8 to 25 carbon atoms, and having carbon atoms Fatty acid amides of 15 to 25 are particularly preferred.
　脂肪酸アミドの具体例としては、オレイン酸アミド、ステアリン酸アミド、エルカ酸アミド、ベヘニン酸アミド、パルミチン酸アミド、ミリスチン酸アミド、ラウリン酸アミド、カプリル酸アミド、カプロン酸アミド、ｎ－オレイルパルミトアミド、ｎ－オレイルエルカアミド、及びそれらの２量体が挙げられる。中でも、オレイン酸アミド、ステアリン酸アミド、エルカ酸アミド、ベヘニン酸アミド、及びそれらの２量体が好ましい。脂肪酸アミドは、１種を単独で用いても良いし、２種以上を併用しても良い。 Specific examples of fatty acid amides include oleic acid amide, stearic acid amide, erucic acid amide, behenic acid amide, palmitic acid amide, myristic acid amide, lauric acid amide, caprylic acid amide, caproic acid amide, n-oleylpalmitamide , N-oleyl erucamide, and their dimers. Among these, oleic acid amide, stearic acid amide, erucic acid amide, behenic acid amide, and dimers thereof are preferable. The fatty acid amide may be used alone or in combination of two or more.
　＜界面活性剤（Ｅ）＞
　本発明に用いる界面活性剤（Ｅ）の種類は特に限定されず、公知の界面活性剤を使用できる。特に、ポリプロピレン系樹脂組成物中において帯電防止剤としての作用を奏する界面活性剤が好ましい。 <Surfactant (E)>
The type of surfactant (E) used in the present invention is not particularly limited, and known surfactants can be used. In particular, a surfactant which exerts an action as an antistatic agent in the polypropylene resin composition is preferable.
　界面活性剤（Ｅ）の代表例としては、エステル型界面活性剤が挙げられる。エステル型界面活性剤としては、炭素原子数８～２５のエステル基を１つ以上有する化合物が好ましく、炭素原子数１５～２５のエステル基を１つ以上有する化合物がより好ましい。これら化合物のエステル基の数は、好ましくは１つ又は２つである。エステル型界面活性剤の具体例としては、グリセリン脂肪酸エステル、ジグリセリン脂肪酸エステル、ソルビタン脂肪酸エステル、ショ糖脂肪酸エステル、アルキルグルコシド、多価カルボン酸エステルが挙げられる。中でも、グリセリン脂肪酸エステル、ジグリセリン脂肪酸エステルが好ましい。 An ester type surfactant is mentioned as a representative example of surfactant (E). As the ester type surfactant, a compound having one or more ester groups having 8 to 25 carbon atoms is preferable, and a compound having one or more ester groups having 15 to 25 carbon atoms is more preferable. The number of ester groups in these compounds is preferably one or two. Specific examples of the ester type surfactant include glycerin fatty acid ester, diglycerin fatty acid ester, sorbitan fatty acid ester, sucrose fatty acid ester, alkyl glucoside, polyvalent carboxylic acid ester. Among them, glycerin fatty acid ester and diglycerin fatty acid ester are preferable.
　グリセリン脂肪酸エステル（すなわち、脂肪酸モノグリセリド）の具体例としては、ステアリン酸モノグリセリド、オレイン酸モノグリセリド、リノレイン酸モノグリセリド、ラウリン酸モノグリセリド、パルミチン酸モノグリセリド、ミリスチン酸モノグリセリド、ベヘン酸モノグリセリド、マルガリン酸モノグリセリドが挙げられる。中でも、ステアリン酸モノグリセリド、オレイン酸モノグリセリドが好ましい。 Specific examples of the glycerin fatty acid ester (ie, fatty acid monoglyceride) include stearic acid monoglyceride, oleic acid monoglyceride, linolenic acid monoglyceride, lauric acid monoglyceride, palmitic acid monoglyceride, myristic acid monoglyceride, behenic acid monoglyceride and margaric acid monoglyceride. Among these, stearic acid monoglyceride and oleic acid monoglyceride are preferable.
　ジグリセリン脂肪酸エステル（すなわち、脂肪酸ジグリセリド）の具体例としては、ステアリン酸ジグリセリド、オレイン酸ジグリセリド、リノレイン酸ジグリセリド、ラウリン酸ジグリセリド、パルミチン酸ジグリセリド、ミリスチン酸ジグリセリド、ベヘン酸ジグリセリド、マルガリン酸ジグリセリドが挙げられる。中でも、ステアリン酸ジグリセリド、オレイン酸ジグリセリドが好ましい。 Specific examples of diglycerin fatty acid esters (ie, fatty acid diglycerides) include stearic acid diglyceride, oleic acid diglyceride, linolenic acid diglyceride, lauric acid diglyceride, palmitic acid diglyceride, myristic acid diglyceride, behenic acid diglyceride, margaric acid diglyceride . Among them, stearic acid diglyceride and oleic acid diglyceride are preferable.
　＜その他の添加剤＞
　本発明のポリプロピレン系樹脂組成物には、必要に応じて、耐熱安定剤、耐候安定剤、耐光安定剤、老化防止剤、酸化防止剤、脂肪酸金属塩、軟化剤、分散剤、着色剤、顔料紫外線吸収剤、核剤などのその他の添加剤を、本発明の目的を損なわない範囲で配合しても良い。 <Other additives>
In the polypropylene resin composition of the present invention, if necessary, heat stabilizers, weather stabilizers, light stabilizers, antioxidants, antioxidants, fatty acid metal salts, softeners, dispersants, colorants, pigments Other additives such as UV absorbers and nucleating agents may be blended within the scope of the purpose of the present invention.
　配合する各成分の混合順序は任意である。各成分を同時に混合しても良いし、一部の成分を混合した後に他の成分を混合する多段階の混合方法を用いても良い。 The order of mixing of the components to be blended is optional. Each component may be mixed simultaneously, or a multistage mixing method may be used in which some components are mixed and then other components are mixed.
　＜ポリプロピレン系樹脂組成物＞
　本発明のポリプロピレン系樹脂組成物においては、以下の方法により測定される、ポリプロピレン系樹脂（Ａ）の粘度［（Ａ）η］が４０～７０Ｐａ・ｓ、エチレン・α－オレフィン共重合体（Ｂ）の粘度［（Ｂ）η］が５０～３３０Ｐａ・ｓであり、それらの比［（Ｂ）η／（Ａ）η］が７.２以下である。
　［粘度の測定方法］
　長さ４０ｍｍ、内径１ｍｍのキャピラリー内で、温度２１０℃、せん断速度１０００／ｓの条件で、キャピラリーから流出する際のポリプロピレン系樹脂（Ａ）及びエチレン・α－オレフィン共重合体（Ｂ）の粘度を測定する。 <Polypropylene-based resin composition>
In the polypropylene resin composition of the present invention, the viscosity [(A)]] of the polypropylene resin (A) measured by the following method is 40 to 70 Pa · s, an ethylene · α-olefin copolymer (B The viscosity [(B)]] is 50 to 330 Pa · s, and their ratio [(B) // (A)]] is 7.2 or less.
[Method of measuring viscosity]
Viscosity of polypropylene resin (A) and ethylene / α-olefin copolymer (B) when flowing out from the capillary at a temperature of 210 ° C. and a shear rate of 1000 / s in a capillary having a length of 40 mm and an inner diameter of 1 mm. Measure
　ポリプロピレン系樹脂（Ａ）の粘度［（Ａ）η］は４０～７０Ｐａ・ｓであり、好ましくは４２～６５Ｐａ・ｓ、より好ましくは４５～５５Ｐａ・ｓである。 The viscosity [(A)]] of the polypropylene resin (A) is 40 to 70 Pa · s, preferably 42 to 65 Pa · s, more preferably 45 to 55 Pa · s.
　エチレン・α－オレフィン共重合体（Ｂ）の粘度［（Ｂ）η］は５０～３３０Ｐａ・ｓであり、好ましくは５０～３００Ｐａ・ｓ、より好ましくは５０～２５０Ｐａ・ｓである。粘度［（Ｂ）η］が適度に低い場合は、引張伸び等の物性が向上する。 The viscosity [(B)]] of the ethylene / α-olefin copolymer (B) is 50 to 330 Pa · s, preferably 50 to 300 Pa · s, more preferably 50 to 250 Pa · s. When the viscosity [(B)]] is appropriately low, physical properties such as tensile elongation are improved.
　ポリプロピレン系樹脂（Ａ）の粘度［（Ａ）η］とエチレン・α－オレフィン共重合体（Ｂ）の粘度［（Ｂ）η］の比［（Ｂ）η／（Ａ）η］は７.２以下であり、好ましくは６.８以下、より好ましくは６.４以下である。 The ratio of the viscosity [(A) A] of the polypropylene resin (A) to the viscosity [(B)]] of the ethylene / α-olefin copolymer (B) [(B) ・ / (A)]] is 7. It is 2 or less, preferably 6.8 or less, more preferably 6.4 or less.
　本発明のポリプロピレン系樹脂組成物は、以下の方法により測定される滑剤（Ｄ）及び界面活性剤（Ｅ）の合計ブリード量が６００μｇ以上であることが好ましい。
　［ブリード量の測定方法］
　ポリプロピレン系樹脂組成物の射出成形体（サイズ：縦２４０ｍｍ、横８０ｍｍ、厚さ３ｍｍ）を温度５０℃の条件で９時間熱処理した後、該射出成形体をジクロロメタン洗浄液１０ｍＬで洗浄し、洗浄後の該洗浄液１０ｍＬを回収して５ｍＬに濃縮したものを試験液とし、該試験液をガスクロマトグラフィーに供し、絶対検量線法により、射出成形体の表面にブリードしていた滑剤（Ｄ）の量（ブリード量）及び射出成形体の表面にブリードしていた界面活性剤（Ｅ）のブリード量を求める。 In the polypropylene resin composition of the present invention, the total bleed amount of the lubricant (D) and the surfactant (E) measured by the following method is preferably 600 μg or more.
[Method of measuring the amount of bleed]
After heat-treating an injection-molded article of polypropylene resin composition (size: length 240 mm, width 80 mm, thickness 3 mm) at a temperature of 50 ° C. for 9 hours, the injection-molded article is washed with 10 mL of a dichloromethane washing solution and washed 10 mL of the washing solution was recovered and concentrated to 5 mL, and the test solution was subjected to gas chromatography, and the amount of the lubricant (D) bled on the surface of the injection molded body by the absolute calibration method. The amount of bleeding) and the amount of bleeding of the surfactant (E) which has been bled on the surface of the injection-molded product are determined.
　滑剤（Ｄ）のブリード量は、好ましくは２８０μｇ以上、より好ましくは３２０μｇ以上、特に好ましくは３６０μｇ以上、最も好ましくは４５０μｇ以上である。 The bleed amount of the lubricant (D) is preferably 280 μg or more, more preferably 320 μg or more, particularly preferably 360 μg or more, and most preferably 450 μg or more.
　界面活性剤（Ｅ）のブリード量は、好ましくは３２０μｇ以上、より好ましくは６００μｇ以上、特に好ましくは６５０μｇ以上、最も好ましくは７００μｇ以上である。 The bleeding amount of the surfactant (E) is preferably 320 μg or more, more preferably 600 μg or more, particularly preferably 650 μg or more, and most preferably 700 μg or more.
　滑剤（Ｄ）及び界面活性剤（Ｅ）の合計ブリード量は、好ましくは６００μｇ以上、より好ましくは８００μｇ以上、特に好ましくは９００μｇ以上である。 The total bleed amount of the lubricant (D) and the surfactant (E) is preferably 600 μg or more, more preferably 800 μg or more, and particularly preferably 900 μg or more.
　以下、本発明のポリプロピレン系樹脂組成物に含まれる各成分の量について説明する。これら各成分の量は成分（Ａ）、（Ｂ）及び（Ｃ）の合計１００質量部を基準とする。 Hereinafter, the amount of each component contained in the polypropylene resin composition of the present invention will be described. The amount of each of these components is based on 100 parts by mass of components (A), (B) and (C) in total.
　ポリプロピレン系樹脂（Ａ）の量は４９～９０質量部であり、好ましくは５０～９０質量部、より好ましくは７０～９０質量部である。 The amount of the polypropylene resin (A) is 49 to 90 parts by mass, preferably 50 to 90 parts by mass, and more preferably 70 to 90 parts by mass.
　エチレン・α－オレフィン共重合体（Ｂ）の量は９～５０質量部であり、好ましくは１０～５０質量部、より好ましくは２０～５０質量部である。 The amount of the ethylene / α-olefin copolymer (B) is 9 to 50 parts by mass, preferably 10 to 50 parts by mass, and more preferably 20 to 50 parts by mass.
　無機充填剤（Ｃ）の量は０質量部以上１０質量部未満である。すなわち無機充填剤（Ｃ）は、本発明のポリプロピレン系樹脂組成物に含まれていても良いし、含まれていなくても良い。無機充填剤（Ｃ）が含まれている場合、その量は１０質量部未満であり、好ましくは０.１質量部以上１０質量部未満、より好ましくは０.２～８質量部である。 The amount of the inorganic filler (C) is 0 parts by mass or more and less than 10 parts by mass. That is, the inorganic filler (C) may or may not be contained in the polypropylene resin composition of the present invention. When the inorganic filler (C) is contained, the amount is less than 10 parts by mass, preferably 0.1 parts by mass or more and less than 10 parts by mass, more preferably 0.2 to 8 parts by mass.
　本発明のポリプロピレン系樹脂組成物は、滑剤（Ｄ）及び界面活性剤（Ｅ）の両方、若しくは一方を含む。 The polypropylene resin composition of the present invention contains both or one of a lubricant (D) and a surfactant (E).
　（i）滑剤（Ｄ）及び界面活性剤（Ｅ）の両方を含む場合：
　滑剤（Ｄ）及び界面活性剤（Ｅ）の各々の量は０.２～０.６質量部であり、好ましくは０.３～０.５質量部である。 (I) When both lubricant (D) and surfactant (E) are contained:
The amount of each of the lubricant (D) and the surfactant (E) is 0.2 to 0.6 parts by mass, preferably 0.3 to 0.5 parts by mass.
　（ii）滑剤（Ｄ）及び界面活性剤（Ｅ）のうちの一方を含む場合：
　滑剤（Ｄ）又は界面活性剤（Ｅ）の量は０.６質量部を超えて１.２質量部以下であり、好ましくは０.７～１.０質量部、より好ましくは０.７～０.９質量部である。 (Ii) When one of lubricant (D) and surfactant (E) is included:
The amount of the lubricant (D) or surfactant (E) is more than 0.6 parts by mass and 1.2 parts by mass or less, preferably 0.7 to 1.0 parts by mass, more preferably 0.7 to It is 0.9 parts by mass.
　以上説明した各成分の配合の順序は任意である。例えば、各成分をバンバリーミキサー、単軸押出機、２軸押出機、高速２軸押出機などの混合装置により混合又は溶融混練することにより、ポリプロピレン系樹脂組成物が得られる。 The order of blending of the components described above is arbitrary. For example, a polypropylene resin composition can be obtained by mixing or melt-kneading each component with a mixing apparatus such as a Banbury mixer, a single screw extruder, a twin screw extruder, or a high speed twin screw extruder.
　＜成形体＞
　本発明のポリプロピレン系樹脂組成物は、成形性に優れているので、様々な成形法に使用できる。本発明の成形体の具体例としては、射出成形体、発泡成形体、射出発泡成形体、押出成形体、ブロー成形体、真空・圧空成形体、カレンダー成形体、延伸フィルム、インフレーションフィルムが挙げられる。特に、射出成形体が好ましい。成形体を製造する場合の成形条件は特に制限されず、公知の条件を採用できる。 <Molded body>
Since the polypropylene resin composition of the present invention is excellent in moldability, it can be used in various molding methods. Specific examples of the molded article of the present invention include injection molded articles, foam molded articles, injection foam molded articles, extrusion molded articles, blow molded articles, vacuum / pressure molded articles, calendar molded articles, stretched films, and inflation films. . In particular, injection molded articles are preferred. The molding conditions in the case of manufacturing a molded object are not particularly limited, and known conditions can be adopted.
　本発明の成形体は、優れた成形性を有する。また、ポリプロピレン系樹脂（Ａ）を含むので十分な剛性を有し、エチレン・α－オレフィン（Ｂ）を含むので十分な耐衝撃性も有する。さらに滑剤（Ｄ）及び／又は界面活性剤（Ｅ）のブリード量が多いので、無機充填剤を含まない又は無機充填剤の含有量が少ない場合であっても、耐足蹴り傷付き性及びその他の表面特性が優れている。 The molded article of the present invention has excellent moldability. In addition, since the polypropylene-based resin (A) is contained, it has sufficient rigidity, and since it contains ethylene / α-olefin (B), it has sufficient impact resistance. Furthermore, since the amount of bleeding of the lubricant (D) and / or the surfactant (E) is large, resistance to scratching and other problems even when the inorganic filler is not contained or the content of the inorganic filler is small. Surface properties are excellent.
　本発明の成形体の用途は、特に限定されない。好適な用途の具体例としては、ドアパネル、ピラートリム、ドアトリム、ドアロアガーニッシュ、インストルメントパネルなどの自動車内外装部材、エンジンルーム周辺部品、その他自動車部品、家電部品、食品容器、飲料容器、医療容器が挙げられる。中でも、自動車内外装部材の用途が好ましく、自動車ドア部材の用途、ピラー部材の用途が特に好ましい。 The application of the molded article of the present invention is not particularly limited. Specific examples of suitable applications include door panels, pillar trims, door trims, door lower garnish, automobile interior and exterior members such as instrument panels, engine room peripheral parts, other automobile parts, home appliance parts, food containers, beverage containers, medical containers It can be mentioned. Among them, applications of automobile interior and exterior members are preferable, and applications of automobile door members and applications of pillar members are particularly preferable.
　以下、実施例に基づいて本発明をさらに具体的に説明する。ただし、本発明はこれらの実施例に限定されるものではない。実施例で使用した各材料は以下の通りである。 Hereinafter, the present invention will be more specifically described based on examples. However, the present invention is not limited to these examples. Each material used in the examples is as follows.
　＜ポリプロピレン系樹脂（Ａ）＞
　「Ａ－１」：プロピレン・エチレンブロック共重合体（プライムポリマー社製、ＭＦＲ（２３０℃、２.１６ｋｇ）＝７０ｇ／１０分、エチレン含量＝４０ｍｏｌ％）
　「Ａ－２」：プロピレン単独共重合体（プライムポリマー社製、商品名Ｊ１３７Ｍ、ＭＦＲ（２３０℃、２.１６ｋｇ）＝３０ｇ／１０分）
　「Ａ－３」：プロピレン単独共重合体（プライムポリマー社製、商品名Ｊ１３Ｂ、ＭＦＲ（２３０℃、２.１６ｋｇ）＝２００ｇ／１０分）
　「Ａ－４」：プロピレン単独共重合体（プライムポリマー社製、商品名Ｊ１３７Ｇ、ＭＦＲ（２３０℃、２.１６ｋｇ）＝３０ｇ／１０分） <Polypropylene resin (A)>
“A-1”: Propylene-ethylene block copolymer (manufactured by Prime Polymer Co., MFR (230 ° C., 2.16 kg) = 70 g / 10 min, ethylene content = 40 mol%)
"A-2": Propylene homopolymer (manufactured by Prime Polymer Co., Ltd., trade name J137M, MFR (230 ° C, 2.16 kg) = 30 g / 10 min)
“A-3”: Propylene homopolymer (manufactured by Prime Polymer Co., Ltd., trade name J13B, MFR (230 ° C., 2.16 kg) = 200 g / 10 min)
“A-4”: Propylene homopolymer (manufactured by Prime Polymer Co., Ltd., trade name J137G, MFR (230 ° C., 2.16 kg) = 30 g / 10 min)
　＜エチレン・α－オレフィン共重合体（Ｂ）＞
　「Ｂ－１」：エチレン・１－オクテン共重合体（ＥＯＲ）（ダウ・ケミカル社製、ＥＮＧＡＧＥ（登録商標）８１００、ＭＦＲ（２３０℃、２.１６ｋｇ）＝２.０ｇ／１０分、エチレン含量＝８０ｍｏｌ％）
　「Ｂ－２」：エチレン・１－オクテン共重合体（ＥＯＲ）（ダウ・ケミカル社製、ＥＮＧＡＧＥ（登録商標）８２００、ＭＦＲ（２３０℃、２.１６ｋｇ）＝９.０ｇ／１０分、エチレン含量＝８０ｍｏｌ％）
　「Ｂ－３」：エチレン・１－オクテン共重合体（ＥＯＲ）（ダウ・ケミカル社製、ＥＮＧＡＧＥ（登録商標）８１３７、ＭＦＲ（２３０℃、２.１６ｋｇ）＝２６ｇ／１０分、エチレン含量＝８０ｍｏｌ％）
　「Ｂ－４」：エチレン・１－オクテン共重合体（ＥＯＲ）（ダウ・ケミカル社製、ＥＮＧＡＧＥ（登録商標）８４０７、ＭＦＲ（２３０℃、２.１６ｋｇ）＝６０ｇ／１０分、エチレン含量＝８０ｍｏｌ％）
　「Ｂ－５」：エチレン・１－ブテン共重合体（ＥＢＲ）（三井化学社製、タフマー（登録商標）、ＭＦＲ（２３０℃、２.１６ｋｇ）＝６０ｇ／１０分、エチレン含量＝８０ｍｏｌ％）
　「Ｂ－６」：エチレン・１－ブテン共重合体（ＥＢＲ）（三井化学社製、タフマー（登録商標）、ＭＦＲ（２３０℃、２.１６ｋｇ）＝６.７ｇ／１０分、エチレン含量＝８０ｍｏｌ％）
　「Ｂ－７」：エチレン・１－ブテン共重合体（ＥＢＲ）（三井化学社製、タフマー（登録商標）、ＭＦＲ（２３０℃、２.１６ｋｇ）＝２.２ｇ／１０分、エチレン含量＝８０ｍｏｌ％） <Ethylene-α-olefin copolymer (B)>
“B-1”: ethylene / 1-octene copolymer (EOR) (manufactured by Dow Chemical Co., ENGAGE (registered trademark) 8100, MFR (230 ° C., 2.16 kg) = 2.0 g / 10 min, ethylene content = 80 mol%)
“B-2”: ethylene 1-octene copolymer (EOR) (manufactured by Dow Chemical Co., ENGAGE (registered trademark) 8200, MFR (230 ° C., 2.16 kg) = 9.0 g / 10 min, ethylene content = 80 mol%)
“B-3”: ethylene / 1-octene copolymer (EOR) (manufactured by Dow Chemical Co., ENGAGE (registered trademark) 8137, MFR (230 ° C., 2.16 kg) = 26 g / 10 min, ethylene content = 80 mol %)
“B-4”: ethylene 1-octene copolymer (EOR) (manufactured by Dow Chemical Co., ENGAGE (registered trademark) 8407, MFR (230 ° C., 2.16 kg) = 60 g / 10 min, ethylene content = 80 mol %)
"B-5": ethylene / 1-butene copolymer (EBR) (manufactured by Mitsui Chemicals, Tafmar (registered trademark), MFR (230 ° C, 2.16 kg) = 60 g / 10 min, ethylene content = 80 mol%)
“B-6”: ethylene / 1-butene copolymer (EBR) (manufactured by Mitsui Chemicals, Tafmar (registered trademark), MFR (230 ° C., 2.16 kg) = 6.7 g / 10 min, ethylene content = 80 mol %)
“B-7”: ethylene / 1-butene copolymer (EBR) (Mitsui Chemical Co., Ltd., Tafmer (registered trademark), MFR (230 ° C., 2.16 kg) = 2.2 g / 10 min, ethylene content = 80 mol %)
　＜無機充填剤（Ｃ）＞
　「Ｃ－１」：タルク（浅田製粉(株)製、商品名ＪＭ－２０９、平均粒径（レーザー回折）４～５μｍ） <Inorganic filler (C)>
“C-1”: Talc (manufactured by Asada Powder Co., Ltd., trade name JM-209, average particle size (laser diffraction) 4 to 5 μm)
　＜滑剤（Ｄ）＞
　「Ｄ－１」：エルカ酸アミド（日本精化社製、ニュートロン（登録商標）Ｓ） <Lubricant (D)>
"D-1": Erucic acid amide (manufactured by Nippon Seika Co., Ltd., Neutron (registered trademark) S)
　＜界面活性剤（Ｅ）＞
　「Ｅ－１」：ステアリン酸モノグリセリド（花王社製、エレクトロストリッパー（登録商標）ＴＳ－５） <Surfactant (E)>
"E-1": stearic acid monoglyceride (manufactured by Kao Corporation, Electro Stripper (registered trademark) TS-5)
　＜実施例１ａ～１０ａ、比較例１ａ～１０ａ＞
　表１～４に示す各成分（質量部）、及び、その他の添加剤として、フェノール系酸化防止剤（ＢＡＳＦ社製、商品名Ｉｒｇａｎｏｘ（登録商標）１０１０）０.１質量部、リン系酸化防止剤（ＢＡＳＦ社製、商品名Ｉｒｇａｆｏｓ１６８）０.０５質量部、ヒンダードアミン系光安定剤（ＡＤＥＫＡ製、商品名ＬＡ－５２）０.０５質量部、紫外線吸収剤（ＢＡＳＦ社製、商品名Ｔｉｎｕｖｉｎ（登録商標）１２０）０.０５質量部、核剤（ＡＤＥＫＡ製、商品名アデカスタブ（登録商標）ＮＡ－１１）０.１質量部を含むポリプロピレン系樹脂組成物を調製した。 Examples 1a to 10a and Comparative Examples 1a to 10a
Each component (parts by mass) shown in Tables 1 to 4 and, as other additives, 0.1 part by mass of a phenolic antioxidant (manufactured by BASF, trade name Irganox (registered trademark) 1010), phosphorus antioxidant Agent (BASF, trade name Irgafos 168) 0.05 parts by weight, hindered amine light stabilizer (ADEKA, trade name LA-52) 0.05 parts by weight, UV absorber (BASF, trade name Tinuvin (registered trademark) A polypropylene resin composition was prepared containing 0.05 parts by mass of a trade mark 120) and 0.1 parts by mass of a nucleating agent (manufactured by ADEKA, trade name Adekastab (registered trademark) NA-11).
　そして、これらポリプロピレン系樹脂組成物の各物性を下記の方法により測定あるいは評価した。結果を表１～３に示す。 And each physical property of these polypropylene resin compositions was measured or evaluated by the following method. The results are shown in Tables 1 to 3.
　［粘度（η）］
　東洋精機製作所製のＣＡＰＩＲＯＧＲＡＰＨ―１Ｄを用いて、長さ４０ｍｍ、内径１ｍｍのキャピラリー内に成分（Ａ）を充填し、温度２１０℃、せん断速度１０００／ｓの条件で、キャピラリーから流出する際の成分（Ａ）の粘度［（Ａ）η］を測定した。また同じ条件で、成分（Ｂ）の粘度［（Ｂ）η］も測定した。そして、これら測定値から両者の比［（Ｂ）η／（Ａ）η］を算出した。 [Viscosity (η)]
Component (A) is filled in a capillary with a length of 40 mm and an inner diameter of 1 mm using CAPIROGRAPH-1D manufactured by Toyo Seiki Seisakusho, and the component when flowing out from the capillary at a temperature of 210 ° C. and a shear rate of 1000 / s. The viscosity [(A)]] of (A) was measured. Further, the viscosity [(B) η] of the component (B) was also measured under the same conditions. And the ratio [(B) eta / (A) eta] of both was computed from these measured values.
　［スカッフ足蹴り試験（ゴム摩擦による耐傷付き性試験）］
　樹脂組成物を金型に射出成形して製造した表面にシボを有する成形体を、成形後１週間以上経過後、試験前に２３℃恒温状態で２時間以上静置して状態調節したものを、テストピース（縦２４０ｍｍ、横８０ｍｍ、厚さ３ｍｍ）として用いた。 [Scuff kick test (scratch resistance test by rubber friction)]
A molded article having a emboss on the surface manufactured by injection molding a resin composition into a mold, which has been conditioned by standing at 23 ° C. under a constant temperature condition for 2 hours or more after 1 week or more after molding , And used as a test piece (240 mm long, 80 mm wide, 3 mm thick).
　評価には、図１に示すスカッフ足蹴り試験装置を用いた。このスカッフ足蹴り試験装置は、テストピース１を固定具（不図示）によって固定する台座３と、摩擦物（ゴム試験片）２を先端に装着した金属製の振り子７とパンタグラフ４を具備する装置である。摩擦物（ゴム試験片）２としては、ショアＡ表面硬度が７５であるゴム片（本田技研工業社製、品番１８２１５－ＳＡ０－０００）を用いた。この装置は、テストピース１の傷付き試験面６から２０ｃｍの高さ５より振り子７を作動させ、振り子７の先端に装着した摩擦物（ゴム試験片）２が、テストピース１の試験面６上を摩擦して通過させることにより、靴底での足蹴り状態を再現するものである。 For the evaluation, a scuff kicking test device shown in FIG. 1 was used. This scuff test device is equipped with a pedestal 3 for fixing a test piece 1 by a fixture (not shown), and a metal pendulum 7 and a pantograph 4 with a friction object (rubber test piece) 2 mounted on the tip. It is. As the friction material (rubber test piece) 2, a rubber piece having a Shore A surface hardness of 75 (manufactured by Honda Motor Co., Ltd., part number 18215-SA0-000) was used. This device operates the pendulum 7 from the scratched test surface 6 of the test piece 1 from the height 5 of 20 cm, and the friction material (rubber test piece) 2 attached to the tip of the pendulum 7 is the test surface 6 of the test piece 1 By rubbing and passing through the top, it is possible to reproduce the state of kicking on the sole.
　具体的には、作業員２人で次の操作手順に従って試験を行った。
　１．テストピース１を装置の台座３上に固定した。
　２．デジタルデップスゲ－ジを振り子７上部にセットし、ゲージの先端を振り子７上部へ当て、ゲージの目盛りが０ｍｍになることを確認した。
　３．パンタグラフ４のレバーを回転させ、台座３を上昇させゲージの目盛りが０.３ｍｍになるよう合せた。
　４．ゴム試験片２を装着した振り子７先端を傷付き試験面６より２０ｃｍの高さ５まで引き上げた。
　５．振り子７を放し、テストピース１の試験面６へゴム試験片２を擦った。 Specifically, the test was conducted according to the following operation procedure by two workers.
1. The test piece 1 was fixed on the pedestal 3 of the apparatus.
2. The digital dip gauge was set on the upper part of the pendulum 7 and the tip of the gauge was placed on the upper part of the pendulum 7 to confirm that the scale of the gauge was 0 mm.
3. The lever of the pantograph 4 was rotated to raise the pedestal 3 so that the scale of the gauge was 0.3 mm.
4. The tip of the pendulum 7 on which the rubber test piece 2 was mounted was pulled up to a height 5 of 20 cm from the scratched test surface 6.
5. The pendulum 7 was released, and the rubber test piece 2 was rubbed against the test surface 6 of the test piece 1.
　そして試験面６の状態を目視にて確認し、以下の基準により評価した。評価結果は等級５が最も良好、等級１が最も不良を表す。
　「１」：摩擦部の表面の白化が著しく目立っていた。
　「２」：摩擦部の表面の白化が目立っていた。
　「３」：摩擦部の表面がやや白化していた。
　「４」：摩擦部にゴムが擦った跡が有ったが、白化は無かった。
　「５」：ゴムが擦った跡も白化も無かった。 And the state of the test surface 6 was confirmed visually, and the following references | standards evaluated. The evaluation results show that grade 5 is the best and grade 1 is the worst.
"1": The whitening of the surface of the friction part was remarkable remarkably.
"2": Whitening of the surface of the friction part was noticeable.
"3": The surface of the friction portion was slightly whitened.
"4": There was a trace that rubber rubbed on the friction part, but there was no whitening.
"5": There was neither a trace which rubber rubbed, nor whitening.
　［ブリード量］
　ポリプロピレン系樹脂組成物の射出成形体（サイズ：縦２４０ｍｍ、横８０ｍｍ、厚さ３ｍｍ）を温度５０℃の条件で９時間熱処理した後、この射出成形体をジクロロメタン洗浄液１０ｍＬで洗浄し、洗浄後の洗浄液１０ｍＬを回収して５ｍＬに濃縮したものを試験液とした。この試験液をガスクロマトグラフィーに供し、絶対検量線法により、射出成形体の表面にブリードしていた滑剤（Ｄ）及び界面活性剤（Ｅ）のブリード量を求めた。 [Bleed amount]
After heat-treating an injection-molded article of polypropylene resin composition (size: length 240 mm, width 80 mm, thickness 3 mm) at a temperature of 50 ° C. for 9 hours, the injection-molded article is washed with 10 mL of a dichloromethane washing solution and washed What was collect | recovered and 10 mL of washing | cleaning liquids were concentrated to 5 mL was made into the test liquid. The test solution was subjected to gas chromatography, and the amount of the lubricant (D) and surfactant (E) bled on the surface of the injection molded body was determined by the absolute calibration method.
　試験装置としては、滑剤（Ｄ）に対してはアジレント・テクノロジー社製の７８９０Ｂ ＧＣ Ｓｙｓｔｅｍ、界面活性剤（Ｅ）に対してはアジレント・テクノロジー社製の６８９０Ｎ ＧＣ Ｓｙｓｔｅｍを使用した。 As a test apparatus, 7890B GC System made from Agilent Technologies for lubricant (D) and 6890N GC System made from Agilent Technologies for surfactant (E) were used.
Figure JPOXMLDOC01-appb-T000001
Figure JPOXMLDOC01-appb-T000001
Figure JPOXMLDOC01-appb-T000002
Figure JPOXMLDOC01-appb-T000002
Figure JPOXMLDOC01-appb-T000003
Figure JPOXMLDOC01-appb-T000003
Figure JPOXMLDOC01-appb-T000004
Figure JPOXMLDOC01-appb-T000004
　表１～４に示す通り、実施例１ａ～１０ａのポリプロピレン系樹脂組成物は、滑剤（Ｄ）及び／又は界面活性剤（Ｅ）のブリード量が高く、耐足蹴り傷付き性が優れていた。 As shown in Tables 1 to 4, in the polypropylene resin compositions of Examples 1a to 10a, the amount of bleeding of the lubricant (D) and / or the surfactant (E) was high, and the resistance to kicking was excellent. .
　一方、比［（Ｂ）η／（Ａ）η］が比較的大きい比較例１ａ～３ａ、５ａ及び６ａのポリプロピレン系樹脂組成物は、滑剤（Ｄ）及び／又は界面活性剤（Ｅ）のブリード量が低く、耐足蹴り傷付き性が劣っていた。また、ゴム成分であるエチレン・α－オレフィン共重合体（Ｂ）を含まない比較例４ａのポリプロピレン系樹脂組成物も、滑剤（Ｄ）及び／又は界面活性剤（Ｅ）のブリード量が低く、耐足蹴り傷付き性が劣っていた。 On the other hand, the polypropylene-based resin compositions of Comparative Examples 1a to 3a, 5a and 6a having relatively large ratios [(B) η / (A) ブ] are bleeds of lubricant (D) and / or surfactant (E). The amount was low and the resistance to kicking was inferior. Also, the polypropylene resin composition of Comparative Example 4a not containing the rubber component ethylene / α-olefin copolymer (B) also has a low amount of bleeding of the lubricant (D) and / or the surfactant (E), Resistance to kicking was inferior.
　無機充填剤（Ｃ）の含有量が多い比較例７ａ～１０ａのポリプロピレン系樹脂組成物は、無機充填剤（Ｃ）によって耐足蹴り傷付き性が改善された。しかし、このような組成物は全体としての比重が高いので軽量化の観点からは好ましくない。 The polypropylene resin compositions of Comparative Examples 7a to 10a having a large content of the inorganic filler (C) were improved in the resistance to kicking by the inorganic filler (C). However, such a composition is not preferable from the viewpoint of weight reduction because the specific gravity of the composition as a whole is high.
　＜実施例１ｂ～１２ｂ、比較例１～５ｂ＞
　表５～７に示すように各成分の量を変更したこと以外は、実施例１ａと同様にしてポリプロピレン系樹脂組成物を調製した。これらポリプロピレン系樹脂組成物の各物性を実施例１ａと同様に測定あるいは評価した。結果を表５～７に示す。 Examples 1b to 12b and Comparative Examples 1 to 5b
A polypropylene resin composition was prepared in the same manner as in Example 1a, except that the amounts of the respective components were changed as shown in Tables 5 to 7. The physical properties of these polypropylene resin compositions were measured or evaluated in the same manner as in Example 1a. The results are shown in Tables 5-7.
Figure JPOXMLDOC01-appb-T000005
Figure JPOXMLDOC01-appb-T000005
Figure JPOXMLDOC01-appb-T000006
Figure JPOXMLDOC01-appb-T000006
Figure JPOXMLDOC01-appb-T000007
Figure JPOXMLDOC01-appb-T000007
　表５～７に示す通り、実施例１ｂ～１０ｂのポリプロピレン系樹脂組成物は、滑剤（Ｄ）及び／又は界面活性剤（Ｅ）のブリード量が高く、耐足蹴り傷付き性が優れていた。 As shown in Tables 5 to 7, in the polypropylene resin compositions of Examples 1b to 10b, the amount of bleeding of the lubricant (D) and / or the surfactant (E) was high, and the resistance to scratching was excellent. .
　一方、比［（Ｂ）η／（Ａ）η］が比較的大きい比較例１ｂ、２ｂ、４ｂ及び５ｂのポリプロピレン系樹脂組成物は、滑剤（Ｄ）及び／又は界面活性剤（Ｅ）のブリード量が低く、耐足蹴り傷付き性が劣っていた。また、ゴム成分であるエチレン・α－オレフィン共重合体（Ｂ）を含まない比較例３ｂのポリプロピレン系樹脂組成物も、滑剤（Ｄ）及び／又は界面活性剤（Ｅ）のブリード量が低く、耐足蹴り傷付き性が劣っていた。 On the other hand, the polypropylene-based resin compositions of Comparative Examples 1b, 2b, 4b and 5b having relatively large ratios [(B) (/ (A) ブ] are bleeds of the lubricant (D) and / or the surfactant (E). The amount was low and the resistance to kicking was inferior. In addition, the polypropylene resin composition of Comparative Example 3b not containing the ethylene / α-olefin copolymer (B) which is a rubber component also has a low bleeding amount of the lubricant (D) and / or the surfactant (E). Resistance to kicking was inferior.
　本発明のポリプロピレン系樹脂組成物は、射出成形体などの各種の成形体を製造する為の材料として有用である。本発明の成形体は、特に、ドアパネル、ピラートリム、ドアトリム、ドアロアガーニッシュ、インストルメントパネルなどの自動車内外装部材として非常に有用である。 The polypropylene resin composition of the present invention is useful as a material for producing various molded articles such as injection molded articles. The molded article of the present invention is very useful particularly as an automobile interior / exterior member such as a door panel, a pillar trim, a door trim, a door lower garnish, an instrument panel and the like.
　１　テストピース
　２　摩擦物（ゴム試験片）
　３　台座
　４　パンタグラフ
　５　振り子の高さ（２０ｃｍ）
　６　試験面
　７　振り子 1 Test piece 2 Friction material (rubber test piece)
3 pedestal 4 pantograph 5 height of pendulum (20 cm)
6 test surface 7 pendulum

Claims (8)

  1. 　ポリプロピレン系樹脂（Ａ）４９～９０質量部、エチレン・α－オレフィン共重合体（Ｂ）９～５０質量部及び無機充填剤（Ｃ）０質量部以上１０質量部未満を含み、
    　さらに、
    （i）滑剤（Ｄ）及び界面活性剤（Ｅ）を各々０.２～０.６質量部、
    若しくは、
    （ii）滑剤（Ｄ）又は界面活性剤（Ｅ）を０.６質量部を超えて１.２質量部以下
    含み、
    ［但し、成分（Ａ）、（Ｂ）及び（Ｃ）の合計を１００質量部とする。］
    　以下の方法により測定される、ポリプロピレン系樹脂（Ａ）の粘度［（Ａ）η］が４０～７０Ｐａ・ｓ、エチレン・α－オレフィン共重合体（Ｂ）の粘度［（Ｂ）η］が５０～３３０Ｐａ・ｓであり、それらの比［（Ｂ）η／（Ａ）η］が７.２以下であるポリプロピレン系樹脂組成物。
    　［粘度の測定方法］
    　長さ４０ｍｍ、内径１ｍｍのキャピラリー内で、温度２１０℃、せん断速度１０００／ｓの条件で、キャピラリーから流出する際のポリプロピレン系樹脂（Ａ）及びエチレン・α－オレフィン共重合体（Ｂ）の粘度を測定する。     49 to 90 parts by mass of a polypropylene resin (A), 9 to 50 parts by mass of an ethylene / α-olefin copolymer (B), and 0 to 10 parts by mass of an inorganic filler (C),
    further,
    (I) 0.2 to 0.6 parts by mass of lubricant (D) and surfactant (E), respectively
    Or
    (Ii) more than 0.6 parts by mass and 1.2 parts by mass or less of a lubricant (D) or surfactant (E),
    [However, the total of components (A), (B) and (C) is 100 parts by mass. ]
    The viscosity [(A)]] of the polypropylene resin (A) is 40 to 70 Pa · s, and the viscosity [(B)]] of the ethylene / α-olefin copolymer (B) is 50 measured by the following method. A polypropylene resin composition which has a ratio of (B) // (A)] of not more than 7.2 and not more than 330 Pa · s.
    [Method of measuring viscosity]
    Viscosity of polypropylene resin (A) and ethylene / α-olefin copolymer (B) when flowing out from the capillary at a temperature of 210 ° C. and a shear rate of 1000 / s in a capillary having a length of 40 mm and an inner diameter of 1 mm. Measure
  2. 　以下の方法により測定される滑剤（Ｄ）及び界面活性剤（Ｅ）の合計ブリード量が６００μｇ以上である請求項１に記載のポリプロピレン系樹脂組成物。
    　［ブリード量の測定方法］
    　ポリプロピレン系樹脂組成物の射出成形体（サイズ：縦２４０ｍｍ、横８０ｍｍ、厚さ３ｍｍ）を温度５０℃の条件で９時間熱処理した後、該射出成形体をジクロロメタン洗浄液１０ｍＬで洗浄し、洗浄後の該洗浄液１０ｍＬを回収して５ｍＬに濃縮したものを試験液とし、該試験液をガスクロマトグラフィーに供し、絶対検量線法により、射出成形体の表面にブリードしていた滑剤（Ｄ）の量（ブリード量）及び射出成形体の表面にブリードしていた界面活性剤（Ｅ）のブリード量を求める。     The polypropylene resin composition according to claim 1, wherein the total bleed amount of the lubricant (D) and the surfactant (E) measured by the following method is 600 μg or more.
    [Method of measuring the amount of bleed]
    After heat-treating an injection-molded article of polypropylene resin composition (size: length 240 mm, width 80 mm, thickness 3 mm) at a temperature of 50 ° C. for 9 hours, the injection-molded article is washed with 10 mL of a dichloromethane washing solution and washed 10 mL of the washing solution was recovered and concentrated to 5 mL, and the test solution was subjected to gas chromatography, and the amount of the lubricant (D) bled on the surface of the injection molded body by the absolute calibration method. The amount of bleeding) and the amount of bleeding of the surfactant (E) which has been bled on the surface of the injection-molded product are determined.
  3. 　滑剤（Ｄ）が脂肪酸アミドである請求項１に記載のポリプロピレン系樹脂組成物。 The polypropylene resin composition according to claim 1, wherein the lubricant (D) is a fatty acid amide.
  4. 　脂肪酸アミドが、炭素原子数８～２５の脂肪酸アミド及びその２量体からなる群より選ばれる１種以上の脂肪酸アミドである請求項３に記載のポリプロピレン系樹脂組成物。 The polypropylene resin composition according to claim 3, wherein the fatty acid amide is one or more fatty acid amides selected from the group consisting of fatty acid amides having 8 to 25 carbon atoms and dimers thereof.
  5. 　界面活性剤（Ｅ）が、炭素原子数８～２５のエステル基を１つ以上有する化合物である請求項１に記載のポリプロピレン系樹脂組成物。 The polypropylene resin composition according to claim 1, wherein the surfactant (E) is a compound having one or more ester groups having 8 to 25 carbon atoms.
  6. 　請求項１に記載のポリプロピレン系樹脂組成物からなる成形体。 The molded object which consists of a polypropylene resin composition of Claim 1.
  7. 　自動車内外装部材である請求項６に記載の成形体。 The molded article according to claim 6, which is an automobile interior / exterior member.
  8. 　自動車ドア部材又はピラー部材である請求項７に記載の成形体。 The molded article according to claim 7, which is an automobile door member or a pillar member.
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