WO2005030867A2

WO2005030867A2 - Thermoplastic resin composition and injection molded articles comprising the same

Info

Publication number: WO2005030867A2
Application number: PCT/JP2004/012907
Authority: WO
Inventors: Satoru Moritomi; Takashi Sanada
Original assignee: Sumitomo Chemical Company, Limited
Priority date: 2003-09-29
Filing date: 2004-08-31
Publication date: 2005-04-07
Also published as: WO2005030867A3

Abstract

A thermoplastic resin composition comprising a propylene-ethylene block copolymer which comprises a propylene homopolymer portion and a propylene-ethylene random copolymer portion, an elastomer, a filler and optionally a polypheylene ether, which has excellent properties such as the balance of rigidity and impact resistance, the appearance of molded articles produced from the thermoplastic resin composition, and fluidity.

Description

DESCRIPTION THERMOPLASTIC RESIN COMPOSITION AND INJECTION MOLDED ARTICLES COMPRISING THE SAME

Technical Field The present invention relates to a thermoplastic resin composition and injection molded articles comprising such a thermoplastic resin composition. In particular, the present invention relates to a thermoplastic resin composition which is excellent in various properties such as the balance of rigidity and impact resistance, the appearance of molded articles produced from the thermoplastic resin composition, fluidity and the like, and inj ectionmolded articles comprising such a thermoplastic resin composition. Background Art The interior and exterior molded parts of automobiles such as bumpers, instrument panels, pillars, fenders and door trims. are required to have high rigidity and high impact resistance. For example, JP-A-5-320446 discloses a resin composition comprising polyphenylene ether and a polyolefin resin as a resin composition with high rigidity and high impact resistance, which is suitable as a material of automobile parts. However, in these years, needs for the reduction of a wall thickness or the increase of a size of a molded article have been increased, and thus the further increase of the rigidity and impact strength of a resin composition has been sought. The resin composition disclosed in JP-A-5-320446 may not satisfy such requirement for the rigidity and impact strength in the case of a molded article having a thinner wall or a bigger size. Disclosure of the Invention An object of the present invention is to provide a thermoplastic resin composition which is excellent in various properties such as the balance of rigidity and impact resistance, the appearance of molded articles produced from the thermoplastic resin composition, fluidity and the like, and injection molded articles comprising such a thermoplastic resin composition. To achieve the above object, the present invention provides the following first to fifth resin compositions: First Resin Composition a thermoplastic resin composition comprising (A) 40 to 85 % by weight of a propylene-ethylene block copolymer which comprises (Al) 95 to 60 % by weight of a propylene homopolymer portion and (A2) 5 to 40 % by weight of a propylene-ethylene random copolymer portion having an ethylene content of 20 to 55 % by weight, (D) 5 to 20 % by weight of an elastomer, (E) 0 to 40 % by weight of a polyphenylene ether resin, (FI) 5 to 12 % by weight of a plate like filler, and (F2) 5 to 12 % by weight of a fibrous filler; Second Resin Composition a thermoplastic resin composition comprising (A) 20 to 70 % by weight of a propylene-ethylene block copolymer which comprises (Al) more than 85 % by weight but not more than 95 % by weight of a propylene homopolymer portion and (A2) not less than 5 % by weight but less than 15 % by weight of a propylene-ethylene random copolymer portion which has an ethylene content of 20 to 50 % by weight and an intrinsic viscosity [η]_Ep of not less than 2 but less than 9 dl/g, (B) 10 to 60 % by weight of a propylene-ethylene block copolymer which comprises (Bl) 50 to 85 % by weight of a propylene homopolymer portion and (B2) 15 to 50 % by weight of a propylene-ethylene random copolymer portion which has an ethylene content of 20 to 50 % by weight and an intrinsic viscosity [T|]_EP of 1 to 4 dl/g, (D) 5 to 25 % by weight of an elastomer, (E) 0 to 40 % by weight of a polyphenylene ether resin, and (F) 10 to 25 % by weight of an inorganic filler; Third Resin Composition a thermoplastic resin composition comprising (A) 35 to 85 % by weight of a propylene-ethylene block copolymer which comprises (Al) 85 to 65 % by weight of a propylene homopolymer portion and (A2) 15 to 35 % by weight of a propylene-ethylene random copolymer portion which has an ethylene content of 20 to 50 % by weight and an intrinsic viscosity [η]κp of not less than 1 but less than 5 dl/g, (B) 5 to 25 % byweight of a propylene-ethylene block copolymer which comprises (Bl ) 85 to 50 % by weight of a propylene homopolymer portion and (B2) 15 to 50 % by weight of a propylene-ethylene random copolymer portion which has an ethylene content of 20 to 50 % by weight and an intrinsic viscosity [η]_Ep of 5 to 10 dl/g, (D) 1 to 25 % by weight of an elastomer, (E) 0 to 40 % by weight of a polyphenylene ether resin, and (F) 9 to 25 % by weight of an inorganic filler; Fourth Resin Composition a thermoplastic resin composition comprising (A) 40 to 85 % by weight of a propylene-ethylene block copolymer which comprises (Al) 95 to 60 % by weight of a propylene homopolymer portion and (A2) 5 to 40 % by weight of a propylene-ethylene random copolymer portion having an ethylene content of 20 to 55 % by weight, (D) 5 to 30 % by weight of an elastomer, (E) 0 to 40 % by weight of a polyphenylene ether resin, and (F) 5 to 15 % by weight of an inorganic filler, wherein X represented by the following formula is at least 30 % by weight :

X = Content of (A) (wt.%) x [Content of (A2) in (A) (wt.%)/100] + Content of (D) (wt.%); Fifth Resin Composition a thermoplastic resin composition comprising (A) 5 to 60 % byweight of a propylene-ethylene block copolymer which comprises (Al ) 95 to 60 % by weight of a propylene homopolymer portion and (A2) 5 to 40 % by weight of a propylene-ethylene random copolymer portion having an ethylene content of 20 to 55 % by weight, (C) 10 to 45 % by weight of a propylene homopolymer having a melt flow rate (MFR) of at least 100 g/10 min. which is measured at 230°C under a load of 21.2 N, (D) 20 to 30 % by weight of an elastomer, (E) 0 to 40 % by weight of a polyphenylene ether resin, (FI) 5 to 15 % by weight of a plate like filler, and (F2) 5 to 15 % by weight of a fibrous filler. In each resin composition, the total of the amounts of the components is 100 % by weight. Furthermore, the present invention provides an injection molded article, preferably an automotive interior or exterior part comprising one of First to Fifth Resin Compositions of the present invention. Best Mode for Carrying Out the Invention Hereinafter, the components contained in each of the thermoplastic resin compositions of the present invention will be explained. (I) Propylene-ethylene block copolymer (A) The propylene-ethylene block copolymer (A) used in the present invention is preferably a copolymer comprising a propylene homopolymer portion (Al) and a propylene-ethylene random copolymer portion (A2) . The block copolymer (A) may be prepared by a per se known method. For example, the propylene homopolymer portion (Al) is prepared in the first step and then the propylene-ethylene random copolymer portion (A2) is prepared in the second step. As apolymerization catalyst, for example, Ziegler catalysts, metallocene catalysts, etc. may be used. The polymerization method may be a slurry polymerization method, a vapor phase polymerization method, etc. -First Resin Composition In the propylene-ethylene block copolymer (A) used in First Resin Composition of the present invention, the weight percentages of the propylene homopolymer portion (Al ) and the propylene-ethylene randomcopolymerportion (A2) are, respectively, 95 to 60 % by weight and 5 to 40 % by weight, preferably 90 to 65 % by weight and 10 to 35 % by weight, more preferably 90 to 70 % by weight and 10 to 30 % by weight, provided that the whole weight of the propylene-ethylene block copolymer (A) is 100 % by weight . When the content of the homopolymer portion (Al) is too large, molded articles produced from the resin composition may have insufficient impact strength. When the content of the homopolymer portion (Al) is too small, molded articles produced from the resin composition may have insufficient rigidity. The ethylene content of the propylene-ethylene random copolymer portion (A2) in the block copolymer (A) is usually from 20 to 55 % by weight, preferably 30 to 55 % by weight, more preferably 30 to 50 % by weight, provided that the whole weight of the propylene-ethylene randomcopolymerportion (A2) is 100 % byweight . When the ethylene content of the propylene-ethylene random copolymer portion (A2) is too large or too small, molded articles produced from the resin composition may have insufficient impact strength. The isotactic pentad fraction of the homopolymer portion (Al) in the block copolymer (A) is preferably at least 0.97, more preferably at least 0.98 from the viewpoint of the rigidity and heat resistance of molded articles produced from the resin composition. The propylene-ethylene random copolymer portion (A2) preferably has an intrinsic viscosity [T|]_EP of 1 to 8 dl/g, more preferably 2 to 7 dl/g from the viewpoint of the balance of rigidity and impact strength of a molded article, the formation of gels and the appearance of a molded article. -Second Resin Composition In the propylene-ethylene block copolymer (A) used in Second Resin Composition of the present invention, the weight percentages of the propylene homopolymer portion (Al) and the propylene-ethylene randomcopolymerportion (A2) are, respectively, more than 85 % by weight but not more than 95 % by weight and not less than 5 % by weight but less than 15 % by weight, preferably more than 85 % by weight but not more than 90 % by weight and not less than 10 % by weight but less than 15 % by weight, provided that the whole weight of the propylene-ethylene block copolymer (A) is 100 % by weight. When the content of the homopolymer portion (Al) is too large, molded articles produced from the resin composition may have insufficient impact strength. When the content of the homopolymer portion (Al) is too small, molded articles produced from the resin composition may have insufficient rigidity. The ethylene content of the propylene-ethylene random copolymer portion (A2) in the block copolymer (A) is usually from 20 to 50 % byweight, preferably 30 to 50 % by weight, more preferably 30 to 45 % by weight, provided that the whole weight of the propylene-ethylene randomcopolymerportion (A2) is 100 %byweight . When the ethylene content of the propylene-ethylene random copolymer portion (A2) is too large or too small, molded articles produced from the resin composition may have insufficient impact strength. The isotactic pentad fraction of the homopolymer portion (Al) in the block copolymer (A) is preferably at least 0.97, more preferably at least 0.98 from the viewpoint of the rigidity and heat resistance of molded articles produced from the resin composition. The propylene-ethylene random copolymer portion (A2) preferably has an intrinsic viscosity [η]_Ep of not less than 2 dl/g but less than 9 dl/g, more preferably not less than 3 dl/g but less than 8 dl/g. When the intrinsic viscosity of the propylene-ethylene random copolymer portion (A2) is too small, the appearance of a molded article may deteriorate. When the intrinsic viscosity is too large, the resin composition may lose its fluidity or the moldability of the composition may deteriorate . -Third Resin Composition In the propylene-ethylene block copolymer (A) used in Third Resin Composition of the present invention, the weight percentages of the propylene homopolymer portion (Al ) and the propylene-ethylene randomcopolymerportion (A2) are, respectively, 85 to 65 % by weight and 15 to 35 % by weight, preferably 90 to 65 % by weight and 10 to 35 % by weight, more preferably 90 to 70 by weight and 10 to 30% by weight, provided that the whole weight of the propylene-ethylene block copolymer (A) is 100 % by weight. When the content of the homopolymer portion (Al ) is too large, molded articles produced from the resin composition may have insufficient impact strength. When the content of the homopolymer portion (Al) is too small, molded articles produced from the resin composition may have insufficient rigidity. The ethylene content of the propylene-ethylene random copolymer portion (A2) in the block copolymer (A) is usually from 20 to 50 % byweight, preferably 30 to 50 % byweight, more preferably 30 to 45 % by weight, provided that the whole weight of the propylene-ethylene randomcopolymerportion (A2) is 100 %byweight . When the ethylene content of the propylene-ethylene random copolymer portion (A2) is too large or too small, molded articles produced from the resin composition may have insufficient impact strength. The isotactic pentad fraction of the homopolymer portion (Al) in the block copolymer (A) is preferably at least 0.97, more preferably at least 0.98 from the viewpoint of the rigidity and heat resistance of molded articles produced from the resin composition. The propylene-ethylene random copolymer portion (A2) preferably has an intrinsic viscosity [η] _EP of not less than 1 dl/g but less than 5 dl/g, more preferably not less than 2 dl/g but less than 4 dl/g. When the intrinsic viscosity of the propylene-ethylene random copolymer portion (A2) is too small, molded articles produced from the resin composition may have in sufficient impact strength. When the intrinsic viscosity is too large, the resincompositionmaylose its fluidityor themoldability of the composition may deteriorate. -Fourth Resin Composition In the propylene-ethylene block copolymer (A) used in Fourth Resin Composition of the present invention, the weight percentages of the propylene homopolymer portion (Al) and the propylene-ethylenerandomcopolymerportion (A2) are, respectevely, 95 to 60 % by weight and 5 to 40 % by weight, preferably 90 to 65 % by weight and 10 to 35 % by weight, more preferably 90 to 70 by weight and 10 to 30% by weight, provided that the whole weight of the propylene-ethylene block copolymer (A) is 100 % by weight. When the content of the homopolymer portion (Al) is too large, molded articles produced from the resin composition may have insufficient impact strength. When the content of the homopolymer portion (Al) is too small, molded articles produced from the resin composition may have insufficient rigidity. The ethylene content of the propylene-ethylene random copolymer portion (A2) in the block copolymer (A) is usually from 20 to 55 % by weight, preferably 30 to 55 % by weight, more preferably 30 to 50 % by weight, provided that the whole weight of the propylene-ethylene randomcopolymerportion (A2) is 100 %byweight . When the ethylene content of the propylene-ethylene random copolymer portion (A2) is too large or too small, molded articles produced from the resin composition may have insufficient impact strength. The isotactic pentad fraction of the homopolymer portion (Al) in the block copolymer (A) is preferably at least 0.97, more preferably at least 0.98 from the viewpoint of the rigidity and heat resistance of molded articles produced from the resin composition. The propylene-ethylene random copolymer portion (A2) preferably has an intrinsic viscosity [η]_Ep of 1 to 8 dl/g, more preferably 2 to 7 dl/g from the viewpoint of the balance of rigidity and impact strength of a molded article, the formation of gels and the appearance of a molded article. -Fifth Resin Composition In the propylene-ethylene block copolymer (A) used in Fifth Resin Composition of the present invention, the weight percentages of the propylene homopolymer portion (Al ) and the propylene-ethylene randomcopolymerportion (A2) are, respectively, 95 to 60 % by weight and 5 to 40 % by weight, preferably 90 to

65 % by weight and 10 to 35 % by weight, more preferably 90 to

70 by weight and 10 to 30% by weight, provided that the whole weight of the propylene-ethylene block copolymer (A) is 100 % by weight. When the content of the homopolymer portion (Al) is too large, molded articles produced from the resin composition may have insufficient impact strength. When the content of the homopolymer portion (Al) is too small, molded articles produced from the resin composition may have insufficient rigidity. The ethylene content of the propylene-ethylene random copolymer portion (A2) in the block copolymer (A) is usually from 20 to 55 % by weight, preferably 30 to 55 % by weight, more preferably 35 to 50 % by weight, provided that the whole weight of the propylene-ethylene randomcopolymerportion (A2) is 100 %byweight . When the ethylene content of the propylene-ethylene random copolymer portion (A2) is too large or too small, molded articles produced from the resin composition may have insufficient impact strength. The isotactic pentad fraction of the homopolymer portion (Al) in the block copolymer (A) is preferably at least 0.97, more preferably at least 0.98, particularly at least 0.985, from the viewpoint of the rigidity and heat resistance of molded articles produced from the resin composition. The propylene-ethylene random copolymer portion (A2 ) preferably has an intrinsic viscosity [η]_EP of 1 to 8 dl/g, more preferably 2 to 7 dl/g from the viewpoint of the balance of rigidity and impact strength of a molded article, the formation of gels and the appearance of a molded article. (II) Propylene-ethylene block copolymer (B) The propylene-ethylene block copolymer (B) used in the present invention is a copolymer comprising a propylene homopolymer portion (Bl) and a propylene-ethylene random copolymer portion (B2) . The propylene-ethylene block copolymer (B) may be prepared by the same method as the preparation method of the propylene-ethylene block copolymer (A) . -Second Resin Composition In the propylene-ethylene block copolymer (B) used in Second Resin Composition of the present invention, the weight percentages of the propylene homopolymer portion (Bl) and the propylene-ethylene randomcopolymerportion (B2) are, respectively, 50 to 85 % by weight and 15 to 50 % by weight, preferably 60 to 85 % by weight and 15 to 40 % by weight, more preferably 70 to 85 by weight and 15 to 30 % by weight, provided that the whole weight of the propylene-ethylene block copolymer (B) is 100 % by weight . When the content of the homopolymer portion (Bl) is too large, the appearance of a molded article produced from the resin composition may deteriorate. When the content of the homopolymer portion (Bl) is too small, molded articles produced from the resin composition may have insufficient rigidity. The ethylene content of the propylene-ethylene random copolymer portion (B2) in the block copolymer (B) is usually from 20 to 50 % by weight, preferably 30 to 50 % by weight, more preferably 30 to 45 % by weight, provided that the whole weight of the propylene-ethylenerandomcopolymerportion (B2) is 100 %byweight . When the ethylene content of the propylene-ethylene random copolymer portion (B2) is too large or too small, molded articles produced from the resin composition may have insufficient impact strength. The isotactic pentad fraction of the homopolymer portion (Bl) in the block copolymer (B) is preferably at least 0.97, more preferably at least 0.98 from the viewpoint of the rigidity and heat resistance of molded articles produced from the resin composition. The propylene-ethylene random copolymer portion (B2) preferably has an intrinsic viscosity [η]_Ep of 1 to 4 dl/g, more preferably 2 to 4 dl/g. When the intrinsic viscosity of the propylene-ethylene random copolymer portion (B2) is too small, the impact resistance of molded articles produced from the resin composition may deteriorate. When the intrinsic viscosity is too large, the resincompositionmaylose its fluidit orthemoldability of the resin composition may deteriorate. -Third Resin Composition In the propylene-ethylene block copolymer (B) used in Third Resin Composition of the present invention, the weight percentages of the propylene homopolymer portion (Bl) and the propylene-ethylene randomcopolymerportion (B2) are, respectively, 85 to 50 % by weight and 15 to 50 % by weight, preferably 80 to 50 % by weight and 20 to 50 % by weight, more preferably 80 to 60 by weight and 20 to 40 % by weight, provided that the whole weight of the propylene-ethylene block copolymer (B) is 100 % by weight. When the content of the homopolymer portion (Bl) is too large, the appearance of a molded article produced from the resin composition may deteriorate. When the content of the homopolymer portion (Bl) is too small, molded articles produced from the resin composition may have insufficient rigidity. The ethylene content of the propylene-ethylene random copolymer portion (B2) in the block copolymer (B) is usually from 20 to 50 % by weight, preferably 30 to 50 % by weight, more preferably 30 to 45 % by weight, provided that the whole weight of the propylene-ethylene randomcopolymerportion (B2) is 100 %byweight . When the ethylene content of the propylene-ethylene random copolymer portion (B2) is too large or too small, molded articles produced from the resin composition may have insufficient impact strength. The isotactic pentad fraction of the homopolymer portion (Bl) in the block copolymer (B) is preferably at least 0.97, more preferably at least 0.98 from the viewpoint of the rigidity and heat resistance of molded articles produced from the resin composition. The propylene-ethylene random copolymer portion (B2) preferably has an intrinsic viscosity [η]_Ep of 5 to 10 dl/g, more preferably 5 to 9 dl/g. When the intrinsic viscosity of the propylene-ethylene random copolymer portion (B2) is too small, the appearance of a molded article produced from the resin composition may deteriorate. When the intrinsic viscosity is too large, the resincompositionmaylose its fluidityor themoldability of the composition may deteriorate. (Ill) Propylene homopolymer (C) The propylene homopolymer (C) used in Fourth Resin Composition may be a similar propylene homopolymer to the homopolymer portion (Al) of the propylene-ethylene block copolymer (A) . The propylene homopolymer (C) has a melt flow rate (MFR) , measured at 230°Cunder 21.2 N, of at least 100 g/10 min. , preferably at least 150 g/10 min., more preferably at least 200 g/10 min. When the MFR is less than 100 g/10 min., the fluidity of the resin compositionmay decrease and, as a result, themoldability of the resin composition may deteriorate. The isotactic pentad fraction of the propylene homopolymer (C) is preferably at least 0.97, more preferably at least 0.98, particularly at least 0.985 from the viewpoint of the rigidity and heat resistance of molded articles produced from the resin composition. [IV) Elastomer (D) The elastomer (D) which is optionally used in the present invention is at least one elastomer selected from the group consisting of (D-l) an aromatic vinyl compound-containing rubber havinga specific gravityof 0.91 or less, (D-2) anethylene-α-olefin random copolymer rubber having a specific gravity of 0.89 or less and (D-3) a propylene-α-olefin random copolymer rubber. Aromatic vinyl compound-containing rubber (D-l) The aromatic vinyl compound-containing rubber (D-l) may be a block copolymer comprising an aromatic vinyl compound polymer block and a conjugated diene polymer block in which preferably, at least 80%, more preferably at least 85% of the double bonds of the conjugated diene polymer block are hydrogenated. The aromatic vinyl compound-containing rubber preferably has a molecular weight distribution (Q value) of 2.5 or less, more preferably 2.3 or less, where the Q value is measured by gel permeation chromatography (GPC) . Preferably, the aromatic vinyl compound-containing rubber contains 10 to 30 % by weight, more preferably 12 to 20 % by weight of the aromatic vinyl compound. Furthermore, the aromatic vinyl compound-containing rubber preferably has a melt flow rate (MFR) , measured according to JIS K 6758 at 230°C, of 1 to 15 g/10 min., more preferably 2 to 13 g/10 min. Specific examples of the aromatic vinyl compound-containing rubber (D-l) include block copolymers such as styrene-ethylene-butylene-styrene rubber (SEBS) , styrene-ethylene-propylene-styrene rubber (SEPS) , styrene-butylene rubber (SBR) , styrene-butadiene-styrene rubber (SBS) and styrene-isoprene-styrene rubber (SIS), each of which may be hydrogenated. In addition, a rubber prepared by reacting anaromaticvinyl compoundsuchas styrenewithanolefiniccopolymer rubber such as ethylene-propylene-non-conjugated diene rubber (EPDM) can be preferably used. Two or more aromatic vinyl compound-containing rubbers may be used in combination. The method for preparing the aromatic vinyl compound-containing rubber is not particularly restricted and may be a method in which an aromatic vinyl compound is bonded to an olefinic copolymer rubber or a conjugated diene rubber by polymerization, reaction, etc. Ethylene-α-olefin random copolymer rubber (D-2) The ethylene-α-olefin random copolymer rubber (D-2) used in the present invention may be any random copolymer rubber comprising ethylene and an α-olefin. The α-olefin is usually an α-olefin having at least 3 carbon atoms, for example, propylene, butene-1, pentene-1, hexene-1, heptene-1, octene-1 and decene, preferably propylene, butene-1, hexene-1 and octene-1. Two or more α-olefins may be used in combination. Specific examples of the ethylene-α-olefin random copolymer rubber (D-2) include an ethylene-propylene random copolymer, an ethylene-butene-1 random copolymer, an ethylene-hexene-1 random copolymer, an ethylene-octene-1 random copolymer, an ethylene-propylene-butene-1 random copolymer, etc. Among them, the ethylene-octene-1 random copolymer, the ethylene-butene-1 random copolymer and the ethylene-hexene-1 random copolymer are preferable. Two or more ethylene-α-olefin random copolymer rubbers may be used in combination. The ethylene-α-olefin randomcopolymer rubber has a specific gravity of 0.89 or less, preferably 0.88 or less, more preferably 0 . 875 or less . The ethylene-α-olefin random copolymer rubber has an MFR (measured at 190°C under 21.2 N) of 0.1 to 40 g/10 min. , preferably 0.5 to 30 g/10 min., more preferably 0.5 to 20 g/10 min. Propylene-α-olefin random copolymer rubber (D-3) The propylene-α-olefin random copolymer rubber (D-3) may be a propylene-butene-1 random copolymer rubber, a propylene-hexene-1 random copolymer rubber, a propylene-octene-1 random copolymer rubber, etc. Among them, the propylene-butene-1 random copolymer rubber is preferable. Two or more propylene-α-olefin random copolymer rubbers may be used in combination. Examples of preferred elastomers (D) used in the present invention include a styrene-ethylene-butene-1-styrene rubber (SEBS) having a specific gravity of 0.90 or less, an ethylene-octene-1 random copolymer having a specific gravity of 0.88 or less and an MFR (190°C, 21.2 N) of 0.5 to 20 g/10 min., and an ethylene-butene-1 random copolymer having a specific gravity of 0.88 or less and an MFR (190°C, 21.2 N) of 0.5 to 20 g/10 min. (V) Polyphenylene ether resin (E) The polyphenylene ether resin (E) optionally used in the present invention may be a polymer or copolymer prepared by oxidatively polymerizing at least one phenol compound of the following formula with oxygen or oxygen-containing gas in the presence of an oxidative coupling catalyst:

wherein Ri, R₂, R₃ R and R₅ independently represent a hydrogen atom, a halogen atom, a hydrocarbon group or a substituted hydrocarbon group, provided that at least one of Ri, R₂, R3, R₄ and R₅ is a hydrogen atom. Specific examples of Ri, R₂, R₃/ R4 and R₅ in the formula include hydrogen, chlorine, fluorine, iodine, methyl, ethyl, n- or iso-propyl, pri-, sec- or tert-butyl, chloroethyl, hydroxyethyl, phenylethyl, benzyl, hydroxymethyl, carboxyethyl, methoxycarbonylethyl, cyanoethyl, phenyl, chlorophenyl, methylphenyl, dimethylphenyl, ethylphenyl, and allyl . Specific examples of the phenol compound represented by the above formula include phenol_N o-, m- or p-cresol, 2,6-, 2,5-, 2,4- or 3, 5-dimethylphenol, 2-methyl-6-phenylphenol, 2, 6-diphenylphenol, 2, 6-diethylphenol, 2-methyl-6-ethylphenol, 2,3,5-, 2,3,6- or 2, 4, 6-trimethylphenol,

3-methyl-6-tert-butylphenol, thymol and 2-methyl-6-allylphenol . Among these compounds, 2, 6-dimethylphenol, 2, 6-diphenylphenol, 3-methyl-6-tert-butylphenol and 2, 3, 6-trimethylphenol are preferable. Furthermore, a phenol compound of a formula other than the above one, e.g. a polyhydroxy aromatic compound such as bisphenol-A, tetrabromobisphenol-A, resorcinol, hydroquinone and novolak resins, may be used as a raw material of a copolymer together with a phenol compound of the above formula. The oxidative coupling catalyst used in the oxidative polymerization of the phenol compound or compounds is not particularly restricted and may be any one having a polymerizability. Methods for the preparation of thepolyphenylene ether resin (E) are disclosed, for example, in US Patent Nos. 3,306,874, 3,306,875 and 3,257,357, the disclosures of which are hereby incorporated by reference, JP-B-52-17880, JP-A-50-51197 and JP-A-1-304119. Specific examples of the polyphenylene ether resin (E) used in the present invention include poly 2, 6-dimethyl-l, 4-phenylene ether) , poly 2, 6-diethyl-l, 4-phenylene ether) , poly 2-methyl-6-ethyl-l, 4-phenylene ether) , poly 2-methyl-6-propyl-l, 4-phenylene ether) , poly 2, 6-dipropyl-l, 4-phenylene ether) , poly 2-ethyl-6-propyl-l, 4-phenylene ether) , poly 2, 6-dibutyl-l, 4-phenylene ether) , poly 2, 6-dipropenyl-l, 4-phenylene ether) , poly 2, 6-dilauryl-l, 4-phenylene ether) , poly 2, 6-diphenyl-l, 4-phenylene ether) , poly 2, 6-dimethoxy-l, 4-phenylene ether) , poly 2, 6-diethoxy-l, 4-phenylene ether) , poly 2-methoxy-6-ethoxy-l, 4-phenylene ether) , poly 2-ethyl-6-stearyloxy-l, 4-phenylene ether) , poly 2-methyl-6-phenyl-l, 4-phenylene ether) , poly 2-methyl-l, 4-phenylene ether), poly 2-ethoxy-l, 4-phenylene ether), poly 2-chloro-l, 4-phenylene ether), poly (3-methyl-6-tert-butyl-l, 4-phenylene ether) , poly (2, 6-dichloro-l, 4-phenylene ether) , poly (2, 5-dibromo-l, 4-phenylene ether) , poly (2, 6-dibenzyl-l, 4-phenylene ether) , and copolymers comprising two or more sorts of repeating units which constitute the above polymers. Also, the polyphenylene ether resin (E) includes copolymers of 2, 6-dimethylphenol with a polysubstituted phenol such as 2, 3, 6-tirimethylphenol, and

2, 3, 5, 6-tetramethylphenol . Among these polyphenylene ether resins, poly (2, 6-dimethyl-l, 4-phenylene ether) and the copolymer of 2, 6-dimethylphenol and 2, 3, 6-tirimethylphenol are preferable . The range of the molecular weight of the polyphenylene ether resin (E) is not uniformly defined since the preferable molecular weight range depends the applications of the resin compositions.

In general, the polyphenylene ether resin (E) has an intrinsic viscosity of 0.1 to 0.7 dl/g, preferably 0.3 to 0.6 dl/g, when measured in chloroform at 30°C. The polyphenylene ether resin (E) used in the present invention may be a modified copolymer obtained by grafting a styrenic compound such as styrene, α-methylstyrene, p-methylstyrene vinyltoluene or chlorostyrene on the above polymer or copolymer. (VI) Filler -Second, Third and Fourth Resin Compositions The kind of the inorganic filler (F) to be contained in

Second, Third and Fourth Resin Compositions according to the present invention is not limited, and any fillers that are used as fillers of conventional thermoplastic resin compositions may be used. Examples of the inorganic filler (F) include talc, mica, calcium carbonate, barium sulfate, magnesium carbonate, clay, alumina, silica, calcium sulfate, magnesium sulfate, magnesium oxysulfate fibers, carbon fibers, glass fibers, metal fibers, wollastonite, whiskers, xonotlite, glass flakes, quartz sand, carbon black, titanium oxide, magnesium hydroxide, zeolites, molybdenum, diatomaceous earth, sericite, SHIRASU (light gray volcanic ash) , calciumhydroxide, calcium sulfite, sodium sulfate, bentonite, graphite, etc. Among them, talc is preferable from the viewpoint of achieving high impact strength of molded articles produced from and the good gloss and appearance of the molded articles . Talc usually has an average particle size of 10 μ or less, preferably 5 μm or less . The average particle size of talc means a 50% equivalent particle size D50, which is obtained from an integral distribution curve of the minus sieve method in which talc is suspended in a liquid medium such as water and alcohol using a centrifugal sedimentation type particlesistribution analyzer . While talc may be used in an untreated form, it may be surface-treated with a conventional coupling agent such as a silane coupling agent or a titanium coupling agent or a surfactant to improve the interfacial adhesion with polypropylene resins and the dispersibility of talc particles in the polypropylene resins. Examples of the surfactant include higher fatty acids, higher fatty acid esters, higher fatty acid amides and higher fatty acid salts. First and Fifth Resin Compositions In First and Fifth Resin Compositions, plate like filler (FI) and fibrous filler (F2) are used as fillers. Plate like filler (FI) means a filler of a scale form and preferably has a ratio of a plate length to a thickness of about

100/1 or more. Specific examples of the plate like filler include talc, mica and glass flakes. Among them, talc is preferable. In this case, the average particle size of talc is the same as that in the case of the filler (F) described above. As in the case of the filler (F) , talc may be used in an untreated form or may be used after being surface-treated with a coupling agent or a surfactant. Fibrous filler (F2) contained in First and Fifth Resin Compositions has a fiber form. Specific examples of the fibrous filler (F2) include magnesium oxysulfate fibers, glass fibers, carbon fibers, metal fibers, wollastonite, whiskers andxonotlite. Among them, magnesium oxysulfate fibers and wollastonite are preferable. In particular, fibrous fillers having a ratio of a major axis length to a minor axis length of at least 2 from the viewpoint of improving rigidity of molded articles. Magnesium oxysulfate fibers to be used in the present invention may for examples, be prepared as follows: A slurry of magnesium oxysulfate fibers in a tangled agglomerated state is prepared by hydrothermal synthesis from a raw material such as magnesium sulfate and magnesium hydroxide or magnesium oxide. Then, the slurry is wet treated with a disperser having a high shearing effect so that the tangled magnesium oxysulfate fibers are disengaged and dispersed, and at the same time, the average length of the fibers is adjusted into the range from 7 to 12 μm by breaking fibers with a length of 20 μm or longer. Thereafter, the fibers are filtrated, dehydrated and dried. The fibers contained in the primary fibers of the magnesium oxysulfate fibers used in the present invention preferably have an average fiber length of 7 to 12 μm from the viewpoint of the rigidity and impact resistance of molded articles produced from the resin composition. The magnesium oxysulfate fibers used in the present invention may be surface treated with waxes such as ontan wax, etc. Such treated magnesium oxysulfate fibers may be produced by the method described in JP-A-2003-73524. Amounts of components Hereinafter, the weight percentage (% by weight) of each component is based on the whole weight of each resin composition (100 % by weight) . (First Resin Composition) The amount of the propylene-ethylene block copolymer (A) contained in First Resin Composition according to the present invention is usually from 40 to 85 % by weight, preferably from 50 to 80 % by weight. One to twenty (1 to 20) % by weight of the block copolymer (A) may be replaced with a propylene homopolymer, which may be the same as the propylene homopolymer constituting the propylene homopolymer portion (Al). The amount of the elastomer (D) contained in First Resin Composition according to the present invention is usually from 5 to 20 % by weight, preferably from 7 to 15 % by weight. When the amount of the elastomer (D) is less than 5 % by weight, molded articles produced from the resin composition may have insufficient impact strength. When. the amount of the elastomer (D) exceeds 20 % by weight, molded articles produced from the resin composition may have insufficient rigidity. First Resin Composition of the present invention may optionally contain the polyphenylene ether (E) in an amount of 0 to 40 % by weight, preferably 0 to 30 % by weight. When the amount of the polyphenylene ether (E) is too large, the chemical resistance of the resin composition may deteriorate . The amount of the plate like filler (FI) contained in First Resin Composition according to the present invention is usually from 5 to 12 % by weight, preferably from 6 to 10 % by weight. When the amount of the plate like filler (FI) is too small, molded articles produced from the resin composition may not have sufficiently improved rigidity. When the amount of the filler (FI) is excessive, the impact strength of molded articles produced from the resin composition may decrease. The amount of the fibrous filler (F2) contained in First Resin Composition according to the present invention is usually from 5 to 12 % by weight, preferably from 5 to 10 % by weight. When the amount of the fibrous filler (F2) is too small, molded articles produced from the resin composition may not have sufficiently improved rigidity. When the amount of the filler (F2) is excessive, the impact strength of molded articles produced from the resin composition may decrease. (Second Resin Composition) The amount of the propylene-ethylene block copolymer (A) contained in Second Resin Composition according to the present invention is usually from 20 to 70 % by weight, preferably from 30 to 60 % by weight. When the amount of the block copolymer (A) is too small, the rigidity of molded articles produced from the resin composition may deteriorate. When the amount of the block copolymer (A) is excessive, the fluidity of the resin composition may decrease. The amount of the propylene-ethylene block copolymer (B) contained in Second Resin Composition according to the present invention is usually from 10 to 60 % by weight, preferably from 10 to 30 % by weight. When the amount of the block copolymer (B) is too small, molded articles produced from the resin composition may not have sufficiently improved impact strength. When the amount of the block copolymer (B) is excessive, the rigidity of molded articles produced from the resin composition may decrease. The amount of the elastomer (D) contained in Second Resin Composition according to the present invention is usually from 5 to 25 % by weight, preferably from 10 to 25 % by weight. When the amount of the elastomer (D) is too small, molded articles produced from the resin composition may not have sufficiently improved impact strength. When the amount of the elastomer (D) is excessive, the rigidity of molded articles produced from the resin composition may decrease. Second Resin Composition of the present invention may optionally contain the polyphenylene ether (E) in an amount of 0 to 40 % by weight, preferably 0 to 30 % by weight. When the amount of the polyphenylene ether (E) is too large, the chemical resistance of the resin composition may deteriorate. The amount of the filler (F) contained in Second Resin Composition according to the present invention is usually from 10 to 25 % by weight, preferably from 10 to 20 % by weight. When the amount of the filler (F) is too small, molded articles produced from the resin composition may not have sufficiently improved rigidity. When the amount of the filler (F) is excessive, the impact strength of molded articles produced from the resin composition may decrease. (Third Resin Composition) The amount of the propylene-ethylene block copolymer (A) contained in Third Resin Composition according to the present invention is usually from 40 to 85 % by weight, preferably from 45 to 75 % by weight. When the amount of the block copolymer (A) is too small, molded articles produced from the resin composition may not have sufficiently improved impact strength.

When the amount of the block copolymer (A) is excessive, the rigidity of molded articles produced from the resin composition may decrease. The amount of the propylene-ethylene block copolymer (B) contained in Third Resin Composition according to the present invention is usually from 5 to 25 % by weight, preferably from 7 to 20 % by weight. When the amount of the block copolymer (B) is too small, a molded article produced from the resin composition may not have sufficiently improved appearance. When the amount of the block copolymer (B) is excessive, the fluidity of the resin composition may decrease. The amount of the elastomer (D) contained in Third Resin Composition according to the present invention is usually from 1 to 25 % by weight, preferably from 5 to 20 % by weight. When the amount of the elastomer (D) is too small, molded articles produced from the resin composition may not have sufficiently improved impact strength. When the amount of the elastomer (D) is excessive, the rigidity of molded articles produced from the resin composition may decrease. Third Resin Composition of the present invention may optionally contain the polyphenylene ether (E) in an amount of 0 to 40 % by weight, preferably 0 to 30 % by weight. When the amount of the polyphenylene ether (E) is too large, the chemical resistance of the resin composition may deteriorate. The amount of the inorganic filler (F) contained in Third Resin Composition according to the present invention is usually from 9 to 25 % by weight, preferably from 10 to 20 % by weight. When the amount of the inorganic filler (F) is too small, molded articles produced from the resin composition may not have sufficiently improved rigidity. When the amount of the inorganic filler (F) is excessive, the impact strength of molded articles produced from the resin composition may decrease. (Fourth Resin Composition) The amount of the propylene-ethylene block copolymer (A) contained in Fourth Resin Composition according to the present invention is usually from 40 to 85 % by weight, preferably from 50 to 80 % by weight. When the amount of the block copolymer (A) is too small, molded articles produced from the resin compositionmay not have sufficiently improved impact resistance . When the amount of the block copolymer (A) is excessive, the rigidity of molded articles produced from the resin composition may decrease. The amount of the elastomer (D) contained in Fourth Resin Composition according to the present invention is usually from 5 to 30 % by weight, preferably from 10 to 30 % by weight. When the amount of the elastomer (D) is too small, molded articles produced from the resin composition may not have sufficiently improved impact strength. When the amount of the elastomer (D) is excessive, the rigidity of molded articles produced from the resin composition may decrease. Fourth Resin Composition of the present invention may optionally contain the polyphenylene ether (E) in an amount of 0 to 40 % by weight, preferably 0 to 30 % by weight. When the amount of the polyphenylene ether (E) is too large, the chemical resistance of the resin composition may deteriorate. The amount of the inorganic filler (F) contained in Fourth Resin Composition according to the present invention is usually from 5 to 15 % by weight, preferably from 7 to 13 % by weight. When the amount of the inorganic filler (F) is too small, molded articles produced from the resin composition may not have sufficiently improved rigidity. When the amount of the inorganic filler (F) is excessive, the impact strength of molded articles produced from the resin composition may decrease. In Fourth Resin Composition of the present invention, X represented by the following formula is at least 30 % by weight: X = Content of (A) (wt.%) x [Content of (A2) in (A) (wt.%)/100] + Content of (D) (wt.%) . When X is too small, molded articles produced from the resin composition may not have sufficiently improved impact strength. When the value X is too large, the rigidity of molded articles produced from the resin composition may decrease. (Fifth Resin Composition) The amount of the propylene-ethylene block copolymer (A) contained in Fifth Resin Composition according to the present invention is usually from 5 to 60 % by weight, preferably from 10 to 55 % by weight. When the amount of the block copolymer (A) is too small, molded articles produced from the resin composition may not have sufficiently improved impact strength. When the amount of the block copolymer (A) is excessive, the rigidity of molded articles produced from the resin composition may decrease. The amount of the propylene homopolymer (C) contained in Fifth Resin Composition according to the present invention is usually from 10 to 45 % by weight, preferably from 15 to 40 % by weight. When the amount of the propylene homopolymer (C) is too small, the fluidity of the resin composition may decrease, or the moldability of the resin compositionmay deteriorate . When the propylene homopolymer (C) is excessive, the impact strength of molded articles produced from the resin composition may decrease. The amount of the elastomer (D) contained in Fifth Resin Composition according to the present invention is usually from 20 to 30 % by weight, preferably from 20 to 28 % by weight. When the amount of the elastomer (D) is too small, molded articles produced from the resin composition may not have sufficiently improved impact strength. When the amount of the elastomer (D) is excessive, the rigidity of molded articles produced from the resin composition may decrease. Fifth Resin Composition of the present invention may optionally contain the polyphenylene ether (E) in an amount of 0 to 40 % by weight, preferably 0 to 30 % by weight. When the amount of the polyphenylene ether (E) is too large, the chemical resistance of the resin composition may deteriorate. The amount of the plate like filler (FI) contained in Fifth Resin Composition according to the present invention is usually from 5 to 15 % by weight, preferably from 7 to 15 % by weight. When the amount of the plate like filler (FI) is too small, molded articles produced from the resin composition may not have sufficiently improved rigidity. When the amount of the plate like filler (FI) is excessive, the impact strength of molded articles produced from the resin composition may deteriorate. The amount of the fibrous filler (F2) contained in Fifth Resin Composition according to the present invention is usually from 5 to 15 % by weight, preferably from 5 to 10 % by weight. When the amount of the fibrous filler (F2) is too small, molded articles produced from the resin composition may not have sufficiently improved rigidity. When the amount of the fibrous filler (F2) is excessive, the impact strength of molded articles produced from the resin composition may deteriorate. Production method of a thermoplastic resin composition In one embodiment, a thermoplastic resin composition of the present invention can be produced by mixing and kneading the components. Examples of the apparatus used for the kneading include a single-screw extruder, a twin-screw extruder, a Banbury mixer and a heat roll. A kneading temperature is usually from 170 to 300° C, and a kneading time is usually from 1 to 20 minutes. All the components may be kneaded at the same time, while the components may be successively charged in the kneading apparatus one by one. When the components are successively charged, the charging order of the components is arbitrary. First to Fourth Resin Compositions may optionally contain a propylene homopolymer. When the propylene homopolymer is compounded in a resin composition, its intrinsic viscosity [η]_P is preferably from 0.7 to 1.2 dl/g. The amount of the propylene homopolymer is preferably from 10 to 60 % by weight based on the whole weight of the resin composition. The thermoplastic resin compositions of the present inventionmaycontainvarious additives such as other thermoplastic resins, antioxidants, UV absorbers, pigments, antistatic agents, copper inhibitors, flame retardants, neutralizing agents, blowing agents, plasticizers, nucleating agents, foam inhibitors, crosslinking agents and lubricants, if desired. The injection molded article of the present invention can be produced by injection molding any of the thermoplastic resin compositions of thepresent inventionby any conventional inj ection molding method. Examples of the applications of the injection molded article of thepresent invention include automotiveparts, parts of electric and electronic appliances, buildingmaterial parts, andpreferably automotive parts such as door trims, body side moldings, fenders, fender guards, side sill garnishes, bumper skirts, aerodynamic spoilers, mudguards, inner panels, pillars, instrument panels and bumpers . First and Fourth Resin Compositions of the present invention are preferably used as interior materials of automobiles such as instrument panels, door trims, inner panels and pillars. Second and Third Resin Compositions of the present invention are preferably used as exterior parts of automobiles such as side braids, fenders, fender guards, side sill garnishes, bumper skirts, aerodynamic spoilers and mudguards. Fifth Resin Composition of the present invention is preferably used as instrument panels, bumper parts, etc. of automobiles. EXAMPLES Hereinafter, the present invention will be illustrated by making reference to Examples and Comparative Examples, which do not limit the scope of the present invention in any way. In Examples and Comparative Examples, physical properties are measured as follows: (1) Melt flow rate (MFR; unit: g/10 min.) A melt flow rate was measured according to ASTM D1238 at a temperature of 230°C under a load of 21.2 N. (2) Flexural modulus (unit: MPa) and flexural strength (unit: MPa) A flexural modulus and a flexural strength were measured according to ASTM D790 at a temperature of 23°C using a specimen having a thickness of 3.2 mm, which was prepared by injection molding. (3) Tensile strength at yield point (unit: MPa) and tensile elongation (unit: %) A tensile strength at yield point and tensile elongation were measured according to ASTM D638 at a temperature of 23 °C using a specimen having a thickness of 3.2 mm, which was prepared by injection molding. (4) Izod impact strength (unit: KJ/m²) A notched Izod impact strength was measured according ASTM D256 at a temperature of 23°C using a specimen having a thickness of 3.2 mm. (5) Appearance A sample piece having a size of 160 mm x 160 mm x 3 mm was produced by injection molding, and the appearance of the sample piece was visually observed and ranked "GOOD" or "NO GOOD". (6) Intrinsic viscosity (unit: dl/g) Using a Ubbelohde viscometer, a reduced viscosity was measured at concentrations of 0.1, 0.2 and 0.5 g/dl. An intrinsic viscosity was obtained by plotting the reduced viscosities against the concentrations and extrapolating the plotted line to a concentration of 0 (zero) . This calculationmethod of an intrinsic viscosity is described in "POLYMER SOLUTIONS, POLYMER EXPERIMENTS 11" (KOBUNSHI YOUEKI, KOUBUNSI JIKKENGAKU 11) , page 491 (published by KYORITSU PUBLISHING Co., Ltd. in 1982) . With polypropylene, tetralin was used as a solvent and the viscosity was measured at 135°C. (7) Molecular weight distribution (Q value) The measurement was carried out by gel permeation chromatography under the following conditions: GPC: Type 150 C manufactured by Waters Column: Shodex 80 MA (two columns) manufactured by Showa Denko K.K. Sample amount: 300 μl (polymer concentration: 0.2 wt.%) Flow rate: 1 ml/min. Temperature: 135°C Solvent: o-dichlorobenzene Using standard polystyrene (manufactured by Tosoh Corporation) , a calibration curve of an elute volume and a molecular weight was prepared. Using this calibration curve, a weight average molecular weight (Mw) and a number average molecular weight (Mn) of a sample polymer, both in terms of polystyrene-converted molecular weights, were found. Then, a Q value (a ratio of Mw to Mn) was calculated. (8) Isotactic pentad fraction (unit: %) An isotactic pentad fraction was measured according to the method described by A. Zambelli, et al . in Macromolecules, _6, 925 (1973) . That is, a ratio of isotactic chains with pentad units in polypropylene chains, that is, a ratio of polypropylene monomer units present at the centers of the chains in which five propylene monomer units are continuously bonded in meso states, was measured using ¹³C-NMR. The assignments of absorption peaks in an NMR spectrumwere carriedout according to the article inMacromolecules 8, 687 (1975) . In concrete terms, an isotactic pentad fraction was obtained in terms as an area fraction of mmmm peaks in the whole peak area of methyl carbon ranges of a ¹³C-NMR spectrum. When an isotactic pentad fraction was measured by the above method with NPL standard material CRM No. M19-14 Polypropylene PP/MWD/2 of the National Physical Laboratory (UK), the fraction was 0.944. (9) A weight ratio of a propylene-ethylene random copolymer portion (A2) to a whole propylene-ethylene block copolymer (A) (Y) ; an ethylene content in a propylene-ethylene random copolymer portion (A2) of a propylene ethylene block copolymer (A) [ (C2')_EP/ % by weight] ; and an ethylene content in a propylene-ethylene block copolymer (A) [(CP'); % by weight] The above properties were calculated from a ¹³C-NMR spectrum measured as described below based on the Report of Kakugo, et al. (Macromolecules, 15, 1150-1152 (1982)) : In a test tube having a diameter of 10 mm, about 200 mg of a propylene-ethylene block copolymer was uniformly dissolved in 3 ml of o-dichlorobenzene to obtain a sample solution, and the sample solutionwas subjected to ¹³C-NMRanalysis under the following conditions : Temperature: 135°C Pulse repeating time: 10 seconds Pulse width: 45° Accumulation number: 2500 times (10) An intrinsic viscosity ([η]_Ep; unit: dl/g) of a propylene-ethylene random copolymer portion (A2) in a propylene-ethylene block copolymer (A) An intrinsic viscosity [η]_Ep of a propylene-ethylene random copolymer portion (A2) in a propylene-ethylene block copolymer (A) was calculated from the intrinsic viscosities of a propylene homopolymer portion (Al) and of the whole block copolymer (A) according to the following equation: [η.EP = [η]τ/Y - ⁽1/Y-l) [η]_P where in [η] _p is an intrinsic viscosity of the propylene homopolymer portion (Al ) , and [η]t is an intrinsic viscosity of the whole block copolymer (A) . To measure the intrinsic viscosity [η]_p of the propylene homopolymer portion (Al) in the propylene-ethylene block copolymer (A) , a propylene homopolymer was sampled just after the first step for preparing a propylene homopolymer portion (Al) in the process for preparing the block copolymer (A) and then the intrinsic viscosity of the sampled polymer was measured. The components used in Examples and Comparative Examples were as follows: (A) Propylene-ethylene block copolymer A-I: Used was AZ 564, a propylene-ethylene block copolymer comprising a propylene homopolymer portion and a propylene-ethylene random copolymer portion, manufactured by Sumitomo Chemical Co., Ltd. Particulars of the block copolymer are as follows: MFR (230°C) : 30 g/10 min., Molecular weight distribution (Q value) of the propylene homopolymer portion: 4.2, Intrinsic viscosity [η]p of the propylene homopolymer portion: 1.05 dl/g, Isotactic pentad fraction of the propylene homopolymer portion:

0.97, Intrinsic viscosity [η]_Ep of the propylene-ethylene random copolymer portion: 4.0 dl/g, the ethylene content (C2' ) _Ep of the propylene-ethylene random copolymer portion: 45% by weight, the content of the propylene-ethylene random copolymer portion in the block copolymer: 16% by weight. A-II

Used was AS 171G, a propylene-ethylene block copolymer comprising a propylene homopolymer portion and a propylene-ethylene random copolymer portion, manufactured by Sumitomo Chemical Co., Ltd.

Particulars of the block copolymer are as follows: MFR (230°C) : 0.9 g/10 min., Molecular weight distribution (Q value) of the propylene homopolymer portion: 4.2, Intrinsic viscosity [η]_P of the propylene homopolymer portion: 2.3 dl/g, Isotactic pentad fraction of the propylene homopolymer portion:

0.97, Intrinsic viscosity [TT _EP of the propylene-ethylene random copolymer portion: 4.5 dl/g, the ethylene content (C2' ) _Ep of the propylene-ethylene random copolymer portion: 37% by weight, the content of the propylene-ethylene random copolymer portion in the block copolymer: 16% by weight. A-III: Used was a propylene-ethylene block copolymer comprising a propylene homopolymer portion and a propylene-ethylene random copolymer portion. The block copolymer was prepared using a catalyst described in JP-A-10-212319 and had the following particulars : MFR (230°C) : 90 g/10 min., Molecular weight distribution (Q value) of the propylene homopolymer portion: 4.0, Intrinsic viscosity [η]_P of the propylene homopolymer portion: 0.8 dl/g, Isotactic pentad fraction of the propylene homopolymer portion:

0.99, Intrinsic viscosity [T|]_EP of the propylene-ethylene random copolymer portion: 6.0 dl/g, the ethylene content (C2^f ) _Ep of the propylene-ethylene random copolymer portion: 40% by weight, the content of the propylene-ethylene random copolymer portion in the block copolymer: 12% by weight. A-IV: Used was a propylene-ethylene block copolymer comprising a propylene homopolymer portion and a propylene-ethylene random copolymer portion. The block copolymer was prepared using a catalyst described in JP-A-10-212319 and had the following particulars : MFR (230°C) : 44 g/10 min., Intrinsic viscosity [η]_P of the propylene homopolymer portion: 0.90 dl/g, Isotactic pentad fraction of the propylene homopolymer portion: 0.99, Intrinsic viscosity [T|]_EP of the propylene-ethylene random copolymer portion: 0.99 dl/g, the ethylene content (C2')_Ep of the propylene-ethylene random copolymer portion: 45% by weight, the content of the propylene-ethylene random copolymer portion in the block copolymer: 27.3% by weight. (B) Propylene-ethylene block copolymer B-I: Used was a propylene-ethylene block copolymer comprising a propylene homopolymer portion and a propylene-ethylene random copolymer portion. The block copolymer was prepared using a catalyst described in JP-A-10-212319 and had the following particulars : Intrinsic viscosity [η]_P of the propylene homopolymer portion: 1.0 dl/g, Intrinsic viscosity [η]_Ep of the propylene-ethylene random copolymer portion: 2.2 dl/g, the ethylene content (C2')_EP of the propylene-ethylene random copolymer portion: 45% by weight, the content of the propylene-ethylene random copolymer portion in the block copolymer: 18% by weight. B-II: Used was a propylene-ethylene block copolymer comprising a propylene homopolymer portion and a propylene-ethylene random copolymer portion. The block copolymer was prepared using a catalyst described in JP-A-10-212319 and had the following particulars : Intrinsic viscosity [η] _P of the propylene homopolymer portion: 0.89 dl/g, Intrinsic viscosity [T|]_EP of the propylene-ethylene random copolymer portion: 7.9 dl/g, the ethylene content (C2')_EP of the propylene-ethylene random copolymer portion: 39% by weight, the content of the propylene-ethylene random copolymer portion in the block copolymer: 25.7% by weight. (C) Propylene homopolymer A propylone homopolymer having a molecular weight distribution (Qvalue) of 4.2 (Mw= 88, 000; Mn= 21, 000) , an intrinsic viscosity [η]_P of 0.77 dl/g, an isotactic pentad fraction of 0.99 and MFR (230°C) of 320 g/10 min. (D) Elastomer D-I: An ethylene-hexene-1 copolymer rubber having a density of 0.870 and an MFR (190°C) of 17 g/10 min., which was prepared at 220°C under 78 MPa using a catalyst described in JP-A-9-87313. D-II: SPO^® N0441 (manufactured by Sumitomo Chemical Co., Ltd.) D-II I: ENGAGE^® 8842 (manufactured by DuPont Dow Elastomers) D-IV: TAFMER^® 4050 (manufactured by Mitsui Chemicals, Inc.). An ethylene-butene-1 copolymer rubber having a specific gravity of 0.86 and an MFR (190°C) of 4 g/10 min. D-V: ENGAGE^® 8200 (manufactured by DuPont Dow Elastomers) . An ethylene-octene-1 copolymer rubber having a specific gravity of 0.870 and an MFR (190°C) of 5 g/10 min. D-VI: TAFMER^® A6050 (manufactured by Mitsui Chemicals, Inc.) . An ethylene-butene random copolymer having an MFR (190°C) of 6 g/10 min. and a specific gravity of 0.863. D-VI I : Tuftec^® H1062 (manufactured by Asahi Kasei Chemicals) . A hydrogenated styrene-butadiene-styrene copolymer having an MFR (230°C) of 4.5 g/10 min. and a specific gravity of 0.89. (E) Polyphenylene ether resin E: A polyphenylene ether having an intrinsic viscosity of 0.40 g/10 min. measured in a chloroform solution (concentration: 0.50 g/dl) at 30°C, which was prepared by homopolymerizing 2, 6-dimethylphenol. (FI) Plate like filler F-I: Talc MWHST^® (talc manufactured by HAYASHI CHEMICALS; average particle size: 2.7 μm) (F2) Fibrous filler F-II: Magnesium oxysulfate fibers Mos-Hige^® A (magnesium oxysulfate manufactured by Ube Material Industries, Ltd.) (G) Other components G-I: Hydrogenated styrene-isoprene-styrene block copolymer SEPTON^® 2104 (manufactured by Kuraray Co., Ltd.; styrene content: 65 % by weight, density: 0.97 g/cm³) G-II: Nucleating agent ADEKASTAB NA-11 (manufactured by Asahi Denka Co., Ltd.) G-III: Lubricant NewS (erucamide manufactured by Nippon Fine Chemical Co., Ltd.) Example 1 The components shown in Table 1 were mixed in the prescribed amounts and charged through a hopper into a twin-screw extruder (TEM 50A manufactured by Toshiba Machine Co., Ltd.), which was set at a cylinder temperature of 260°C and a screw revolution speed of 200 rpm, and the mixture was melt kneaded and extruded into strands. Then, the strands were cut to obtain pellets of a resin composition. The pellets were molded using an injection molding machine (IS 100EN manufactured by Toshiba Machine Co. , Ltd.) at a cylinder temperature of 260°C and a mold temperature of 50°C to produce specimens. Using those specimens, a flexural modulus, a flexural strength and an Izod impact strength were measured. The results are shown in Table 1. Example 2 The components shown in Table 1 were mixed in the prescribed amounts and charged through a hopper into a twin-screw extruder (TEM 50A manufactured by Toshiba Machine Co., Ltd.), which was set at a cylinder temperature of 200°C and a screw revolution speed of 200 rpm, and the mixture was melt kneaded and extruded into strands. Then, the strands were cut to obtain pellets of a resin composition. The pellets were molded with an injection molding machine (IS 100EN manufactured by Toshiba Machine Co . , Ltd.) at a cylinder temperature of 230°C and a mold temperature of 30°C to produce specimens. Using those specimens, a flexural modulus, a flexural strength and an Izod impact strength were measured. The results are shown in Table 1. Comparative Example 1 The experiment was carriedout in the samemanner as inExample 1 except that the components shown in Table 1 were used in the prescribed amounts. The results are shown in Table 1. Table 1

As can be seen from the results of Table 1, the products of Examples 1 and 2, which satisfied the requirements of the present invention, had the excellent flexural modulus and flexural strength, while the product of Comparative Example 1, which did not contain a fibrous filler (F2), had low flexural modulus and flexural strength. Example 3 Specimens were produced in the same manner as in Example 1 except that the components shown in Table 2 were used in the prescribed amounts, and then a tensile strength at yield point, a tensile elongation and an Izod impact strength were measured. The results are shown in Table 2. Example 4 Specimens were produced in the same manner as in Example 2 except that the components shown in Table 2 were used in the prescribed amounts, and then a tensile strength at yield point, a tensile elongation and an Izod impact strength were measured. The results are shown in Table 2. Comparative Example 2 The experiment was carriedout in the samemanner as inExample 3 except that the components shown in Table 2 were used in the prescribed amounts. The results are shown in Table 2. Table 2

As can be seen from the results of Table 2, the products of Examples 3 and 4, which satisfied the requirements of the present invention, had an excellent impact sterngth, while the product ofComparative Example 2 , whichdidnot contain apropylene-ethylene block copolymer (B) , had a low impact strength. Example 5 Specimens were produced in the same manner as in Example 1 except that the components shown in Table 3 were used in the prescribedamounts, and then a flexuralmodulus, a flexural strength, and an Izod impact strength were measured, and the appearance of a molded article was evaluated. The results are shown in Table 3. Example 6 Specimens were produced in the same manner as in Example 2 except that the components shown in Table 3 were used in the prescribedamounts, and then a flexuralmodulus, a flexural strength, and an Izod impact strength were measured, and the appearance of a molded article was evaluated. The results are shown in Table 3. Comparative Example 3 The experiment was carried out in the same manner as inExample 5 except that the components shown in Table 3 were used in the prescribed amounts. The results are shown in Table 3. Table 3

As can be seen from the results of Table 3, the products of Examples 5 and 6, which satisfied the requirements of the present invention, had an excellent impact resistance and good appearance, while the product of Comparative Example 3, which did not contain a propylene-ethylene block copolymer (B) , had a low impact resistance and unsatisfactory appearance. Example 7 Specimens were produced in the same manner as in Example 1 except that the components shown in Table 4 were used in the prescribed amounts, and then an Izod impact strength were measured at 23°C and -30°C. The results are shown in Table 4. Example 8 Specimens were produced in the same manner as in Example 2 except that the components shown in Table 4 were used in the prescribed amounts, and then an Izod impact strength were measured at 23°C and -30°C. The results are shown in Table 4. Comparative Example 4 The experiment was carried out in the samemanner as inExample 7 except that the components shown in Table 4 were used in the prescribed amounts. The results are shown in Table 4. Table 4

As can be seen from the results of Table 4, the products of Examples 7 and 8, which satisfied the requirements of the present invention, had an excellent impact strength, while the product of Comparative Example 4, which had a too small sum of (A2) and (D) (= X) , had a low impact strength. Example 9 Specimens were produced in the same manner as in Example 1 except that the components shown in Table 5 were used in the prescribed amounts, and then a tensile strength at yield point, a tensile elongation and an Izod impact strength were measured. The results are shown in Table 5. Example 10 Specimens were produced in the same manner as in Example 2 except that the components shown in Table 5 were used in the prescribed amounts, and then a tensile strength at yield point, a tensile elongation and an Izod impact strength were measured. The results are shown in Table 5. Comparative Example 5 The experimentwas carriedout in the samemanner as inExample 9 except that the components shown in Table 5 were used in the prescribed amounts. The results are shown in Table 5. Table 5

As can be seen from the results of Table 5, the products of Examples 9 and 10, which satisfied the requirements of the present invention, had a high tensile strength at yield point, and good balance of rigidity and impact resistance, while the product of Comparative Example 5, which did not contain a fibrous filer (F2) , had a slightly low tensile strength at yield point, and lacked balance of rigidity and impact resistance.

Claims

CLAIMS 1. A thermoplastic resin composition comprising (A) 40 to 85 % by weight of a propylene-ethylene block copolymer which comprises (Al) 95 to 60 % by weight of a propylene homopolymer portion and (A2) 5 to 40 % by weight of a propylene-ethylene random copolymer portion having an ethylene content of 20 to 55 % by weight, (D) 5 to 20 % by weight of an elastomer, (E) 0 to 40 % by weight of a polyphenylene ether resin, (FI) 5 to 12 % by weight of a plate like filler, and (F2) 5 to 12 % by weight of a fibrous filler; 2. A thermoplastic resin composition comprising (A) 20 to 70 % by weight of a propylene-ethylene block copolymer which comprises (Al) more than 85 % by weight but not more than 95 % by weight of a propylene homopolymer portion and (A2) not less than 5 % by weight but less than 15 % by weight of a propylene-ethylene random copolymer portion which has an ethylene content of 20 to 50 % by weight and an intrinsic viscosity [η]_Ep of not less than 2 dl/g but less than 9 dl/g, (B) 10 to 60 % by weight of a propylene-ethylene block copolymer which comprises (Bl) 50 to 85 % by weight of a propylene homopolymer portion and (B2) 15 to 50 % by weight of a propylene-ethylene random copolymer portion which has an ethylene content of 20 to 50 % by weight and an intrinsic viscosity [η]_EP of 1 to 4 dl/g, (D) 5 to 25 % by weight of an elastomer, (E) 0 to 40 % by weight of a polyphenylene ether resin, and (F) 10 to 25 % by weight of an inorganic filler; 3. A thermoplastic resin composition comprising (A) 35 to 85 % by weight of a propylene-ethylene block copolymer which comprises (Al) 85 to 65 % by weight of a propylene homopolymer portion and (A2) 15 to 35 % by weight of a propylene-ethylene random copolymer portion which has an ethylene content of 20 to 50 % by weight and an intrinsic viscosity [η]_Ep of not less than 1 dl/g but less than 5 dl/g, (B) 5 to 25 % byweight of a propylene-ethylene block copolymer which comprises (Bl ) 85 to 50 % by weight of a propylene homopolymer portion and (B2 ) 15 to 50 % by weight of a propylene-ethylene random copolymer portion which has an ethylene content of 20 to 50 % by weight and an intrinsic viscosity [η]_Ep of 5 to 10 dl/g, (D) 1 to 25 % by weight of an elastomer, (E) 0 to 40 % by weight of a polyphenylene ether resin, and (F) 9 to 25 % by weight of an inorganic filler; 4. A thermoplastic resin composition comprising (A) 40 to 85 % by weight of a propylene-ethylene block copolymer which comprises (Al) 95 to 60 % by weight of a propylene homopolymer portion and (A2) 5 to 40 % by weight of a propylene-ethylene random copolymer portion having an ethylene content of 20 to 55 % by weight, (D) 5 to 30 % by weight of an elastomer, (E) 0 to 40 % by weight of a polyphenylene ether resin, and (F) 5 to 15 % by weight of an inorganic filler, wherein X represented by the following formula is at least 30 % by weight:

X = Content of (A) (wt.%) x [Content of (A2) in (A) (wt.%)/100] + Content of (D) (wt.%) ; 5. A thermoplastic resin composition comprising (A) 5 to 60 % byweight of a propylene-ethylene block copolymer which comprises (Al ) 95 to 60 % by weight of a propylene homopolymer portion and (A2) 5 to 40 % by weight of a propylene-ethylene random copolymer portion having an ethylene content of 20 to 55 % by weight, (C) 10 to 45 % by weight of a propylene homopolymer having a melt flow rate (MFR) of at least 100 g/10 min. which is measured at 230°C under a load of 21.2 N, (D) 20 to 30 % by weight of an elastomer, (E) 0 to 40 % by weight of a polyphenylene ether resin, (FI) 5 to 15 % by weight of a plate like filler, and (F2) 5 to 15 % by weight of a fibrous filler. 6. An injection molded article comprising a thermoplastic resin composition according to any one of claims 1 to 5. 7. The injection molded article according to claim 6, which is an automotive interior part.