||||||||||||||| USOO559004A United States Patent (19) 11 Patent Number: 5,159,004 Furuta et al. (45. Date of Patent: Oct. 27, 1992 54, THERMOPLASTIC RESIN COMPOSITION 59-126460 7/1984 Japan. 75) Inventors: Motonobu Furuta, Tsukuba; Takashi OTHER PUBLICATIONS Maruyama, Kobe; Hiroyuki Harada, Kirk-Othmer Encyclopedia of Chemical Technology, Ichihara, all of Japan Third Edition, vol. 17. 73) Assignee: Sumitomo Chemical Company, Primary Examiner-Jacob Ziegler Limited, Osaka, Japan Attorney, Agent, or Firm-Birch, Stewart, Kolasch and 21 Appl. No.: 437,894 Birch 22 Filed: Nov. 17, 1989 57) ABSTRACT (30) Foreign Application Priority Data Disclosed herein is a thermoplastic resin composition Nov. 18, 1988 JP Japan ................................ 63-292080 which comprises: Dec. 15, 1988 JP Japan ............. ... 63-314863 (a) polyphenylene ether or a composition containing Mar. 13, 1989 JP Japan .................................. -060319 polyphenylene ether, 51 Int. Cl......................... C08K 5/01; C08K 51/04; (b) (i) a modified propylene polymer grafted with a C08K 53/02; C08K 71/12 styrene-based monomer or a mixture of a styrene 52 U.S. Cl. .................................... 524/390; 524/504; based monomer and a monomer copolymerizable 524/506; 524/508: 525/63; 525/68; 525/70, with the styrene-based monomer, or (ii) a composi 525/92; 525/93; 525/905 tion containing said modified propylene polymer and 58 Field of Search ..................... 525/68, 92,93, 905, a propylene polymer, 525/70; 524/508, 490, 504,506 (c) a rubbery substance, and at least one component selected from the following three components; 56 References Cited (d) a styrene resin having a melt index of 8 or above (at U.S. PATENT DOCUMENTS 250 C. under a load of 5 kg), 3,639,499 2/1972 Snodgrass et al. (e) a low-molecular weight hydrocarbon resin, and 4,102,850 7/1978 Cooper et al. (f) white oil and/or liquid paraffin. 4,483,958 11/1984 Kosaka et al. This thermoplastic resin composition exhibits not only 4,863,997 9/1989 Shibuya et al. ..................... 525/905 good moldability but also well-balanced physical prop FOREIGN PATENT DOCUMENTS erties and heat resistance, and can be easily processed 01422166 5/1985 European Pat. Off. into molded articles having outstanding physical prop 47-336 2/1972 Japan . eities. 51-73560 6/1976 Japan . 54-148836 11/1979 Japan. 18 Claims, No Drawings 5,159,004 1. 2 rates the appearance and mechanical properties of the THERMOPLASTIC RESIN COMPOSITION molded articles. The compatibility of polyphenylene ether with poly BACKGROUND OF THE INVENTION propylene may be improved by incorporating poly 1. Field of the Invention phenylene ether with a propylene polymer grafted with The present invention relates to a novel thermoplas a styrene monomer, as disclosed in Japanese Patent tic resin composition which can be made into molded Laid-open No. 75663/1974. This method, however, articles by injection molding, extrusion molding, or the does not provide any composition which is superior in like. both heat resistance and impact resistance. 10 A resin composition having superior mechanical 2. Related Art properties can be obtained by the incorporation of poly Polyphenylene ether is a resin which is generally phenylene ether with a styrene monomer-grafted prop superior in heat resistance, hot water resistance, dimen ylene polymer and a rubbery substance, as disclosed in sional stability, and mechanical and electrical proper Japanese Patent Application No. 33445/1988. How ties. On the other hand, it suffers from the disadvantage 15 ever, it gives injection molded products which suffer of having poor moldability (due to high melt viscosity), segregation presumably on account of poor melt-flow low chemical resistance, and low impact resistance. characteristics. It is known that polyphenylene ether will have im Under these circumstances, there has been a strong proved moldability without any adverse effect on its demand for a composition composed of polyphenylene superior characteristics when it is decreased in melt 20 ether, modified propylene polymer, and rubber sub viscosity by the incorporation of a polystyrene resin. stance, said composition having good mechanical prop However, the resulting composition is still poor in erties and giving injection molded articles with a good chemical resistance. appearance. It is disclosed in U.S. Pat. No. 418941 and UK Pa tent No. 1344729 that a polyphenylene ether resin com In view of the forgoing, the present inventors carried position will have improved processability when it is 25 out extensive studies to develop a new technology. As decreased in molding temperature and melt viscosity by the result, they succeeded in the production of a new the incorporation of a low-molecular weight hydrocar resin composition which is superior in heat resistance, bon resin. melt-flow characteristics, processability, chemical resis Also, Japanese Patent Laid-open No. 1 18956/1980 tance, appearance, and gloss. This success led to the discloses the incorporation of a petroleum-derived low 30 present invention. molecular weight resin or rosin resin into a polyphenyl SUMMARY OF THE INVENTION ene ether resin composition for the reduction of its melt Accordingly, it is an object of the present invention viscosity. to provide a thermoplastic resin composition which Japanese Patent Publication No. 13584/1982 dis 35 comprises: closes a method of decreasing the melt viscosity of (a) polyphenylene ether or a composition containing polyphenylene ether by incorporation with an aromatic polyphenylene ether, hydrocarbon resin derived from cracked naphtha. (b) (i) a modified propylene polymer grafted with a Although the above-cited inventions are intended to styrene-based monomer or a mixture of a styrene improve the flowability of polyphenylene ether resin based monomer and a monomer copolymerizable compositions, they achieve their object only with a with the styrene-based monomer, or (ii) a composi great sacrifice in heat resistance. Also, they were not tion containing said modified propylene polymer and able to improve the chemical resistance of polyphenyl a propylene polymer, ene ether resin compositions. (c) a rubbery substance, and at least one component Meanwhile, propylene polymers have been in general 45 selected from the following three components; use for the production of molded articles, film, and (d) a styrene resin having a melt index of 8 or above (at sheet on account of their outstanding moldability, 250° C. under a load of 5 kg), toughness, water resistance, and chemical resistance, (e) a low-molecular weight hydrocarbon resin, and and their low price attributable to their low specific (f) white oil and/or liquid paraffin. gravity. 50 It is another object of the present invention to pro Unfortunately, propylene polymers have shortcom vide a thermoplastic resin composition which com ings or room for improvement in heat resistance, stiff prises: ness, impact resistance, coatability, and adhesion prop (a) polyphenylene ether or a composition containing erties. This prevents the development of their new ap polyphenylene ether, plications. There is an urgent need for improvement 55 (b) (i) a modified propylene polymer grafted with a particularly in heat resistance and impact resistance. styrene-based monomer or a mixture of a styrene For this reason, there is a demand for a resin composi based monomer and a monomer copolymerizable tion composed of polyphenylene ether and a propylene with the styrene-based monomer, or (ii) a composi polymer which would exhibit the features of both (i.e., tion containing said modified propylene polymer and improved moldability and improved impact resistance). a propylene polymer, It will find uses in new broad application areas. (c) a rubbery substance, and at least one component In practice, however, no satisfactory resin composi selected from the following three components; tions have been obtained from polyphenylene ether and styrene resin having a melt index of 8 or above (at 250 polypropylene mixed together on account of their poor C. under a load of 5 kg), compatibility. It is only possible to obtain a resin com 65 (e) a low-molecular weight hydrocarbon resin, and position which gives injection molded articles with (f) white oil and/or liquid paraffin, phase separation between polyphenylene ether and the ratio of component (a) to component (b) being 1-90 polypropyiene. This phase separation greatly deterio wt.% to 99-10 wt.%, the amount of component (c) being 5,159,004 3 4. 1-50 parts by weight for 100 parts by weight of the total (a) polyphenylene ether or a composition containing amount of components (a) and (b), and the total amount polyphenylene ether, of components (d), (e), and (f) being 0.1-50 parts by (b) (i) a modified propylene polymer grafted with a weight for 100 parts by weight of the total amount of styrene-based monomer or a mixture of a styrene components (a), (b), and (c). 5 based monomer and a monomer copolymerizable It is further another object of the present invention to with the styrene-based monomer, or (ii) a composi provide a thermoplastic resin composition which com tion containing said modified propylene polymer and prises: a propylene polymer, (a) polyphenylene ether or a composition containing (c) a rubbery substance, and polyphenylene ether, 10 (e) a low-molecular weight hydrocarbon resin, (b) (i) a modified propylene polymer grafted with a the ratio of component (a) to component (b) being 1-90 styrene-based monomer or a mixture of a styrene wt % to 99-10 wt.%, the amount of component (c) being based monomer and a monomer copolymerizable 1-50 parts by weight for 100 parts by weight of the total with the styrene-based monomer, or (ii) a composi amount of components (a) and (b), and the amount of tion containing said modified propylene polymer and 15 component (e) being 0.1-50 parts by weight for 100 a propylene polymer, parts by weight of the total amount of components (a), (c) a rubbery substance, and the following two compo (b), and (c).