Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Mixing of two or more solid polymers; mixing of solid...
Reexamination Certificate
2001-04-20
2003-04-15
Mullis, Jeffrey (Department: 1711)
Synthetic resins or natural rubbers -- part of the class 520 ser
Synthetic resins
Mixing of two or more solid polymers; mixing of solid...
C525S069000, C525S09200D, C525S09200D
Reexamination Certificate
active
06548598
ABSTRACT:
BACKGROUND OF THE INVENTION
The present invention relates to a thermoplastic resin composition comprising a polyolefin resin, a polyphenylene ether-based resin and a hydrogenated block copolymer with a specific structure, and exhibiting excellent tensile elongation, rigidity, impact resistance and heat resistance.
Polyphenylene ether-based resins are used in a variety of fields thanks to their high rigidity and excellent heat resistance and moldability, as well as relatively low cost among engineering plastics. Their drawback, however, is inferior impact resistance.
One method used as means of solving this problem is to blend cheap and highly impact resistant polyolefin resins with polyphenylene ether-based resins, but because polyphenylene ether-based resins and polyolefin resins are poorly compatible, the materials obtained by simple blending thereof have notably inferior properties such as lower impact resistance and interlayer peeling.
Various compositions have been studied which involve addition of styrene-based hydrogenated elastomers as compatibilizers, for the purpose of improving the compatibility between polyphenylene ether-based resins and polyolefin resins (see, for example, U.S. Pat. No. 4,166,055, U.S. Pat. No. 4,239,673, U.S. Pat. No. 4,383,082, European Patent Disclosure 115712, Japanese Unexamined Patent Publication No. Hei 5-320471, Japanese Unexamined Patent Publication No. Hei 6-16924, Japanese Unexamined Patent Publication No. Hei 6-57130, Japanese Unexamined Patent Publication No. Hei 9-241499, Japanese Unexamined Patent Publication No. Hei 9-302167, and the like.)
In particular, Japanese Unexamined Patent Publication No. Hei 9-302167 discloses a resin composition with excellent impact resistance and heat resistance by limiting the vinyl content of the conjugated diene block copolymers to 56-80% before hydrogenation of hydrogenated block copolymers.
However, conventionally used compatibilizers have not always provided sufficient enhancement of the properties of compositions, such as impact resistance, heat resistance, rigidity and resistance to interlayer peeling.
SUMMARY OF THE INVENTION
It is an object of the present invention to provide a resin composition comprising a polyphenylene ether-based resin and a polyolefin resin, which composition has no interlayer peeling and exhibits excellent heat resistance and dynamic properties such as impact resistance, rigidity and tensile breaking elongation, and especially excellent tensile breaking elongation.
A resin composition obtained according to the invention, by improved compatibility between the polyphenylene ether-based resin and polyolefin resin due to addition of a hydrogenated block copolymer with a specific structure, has excellent impact resistance, rigidity, heat resistance, tensile breaking elongation and interlayer peeling resistance, and can therefore be used as a material for various types of molded articles.
It may be used in the fields of food wrapping containers, trays, sheets, tubes, films, fibers, laminates, coating materials, electric and electronic parts such as connectors and printed circuit boards, chassis f or OA devices and household appliances such as computers, and industrial parts such as automobile parts, precision parts and construction materials.
DETAILED DESCRIPTION OF THE INVENTION
The present invention will now be explained in greater detail.
The polyphenylene ether-based resin used as component (i) for the invention may be a homopolymer or a copolymer which has a unit represented by the following formula as its main structural unit.
(where R
1
, R
2
, R
3
and R
4
may be the same or different and each is hydrogen, a halogen, a primary or secondary alkyl group of 1-7 carbons, a phenyl group, a haloalkyl group, an aminoalkyl group, an oxyhydrocarbon group or an oxyhalohydrocarbon group wherein at least two of the carbon atoms separated a halogen atom from oxygen atom).
The reduced viscosity of the polyphenylene ether-based resin (measured at a concentration of 0.5 g/dl in a chloroform solvent at 30° C.) is preferably in the range of 0.15-2 dl/g, and more preferably in the range of 0.2-1 dl/g.
As specific examples of polyphenylene ether-based resins there may be mentioned poly(2,6-dimethyl-1,4-phenylene ether), poly(2-methyl-6-ethyl-1,4-phenylene ether), poly(2-methyl-6-phenyl-1,4-phenylene ether) and poly(2,6-dichloro-1,4-phenylene ether). There may also be mentioned polyphenylene ether copolymers typical of which are copolymers of 2-6-dimethylphenol with other phenols (for example, 2,3,6-trimethylphenol and 2-methyl-6-butylphenol). Preferred among them are copolymers of poly(2,6-dimethyl-1,4-phenylene ether), 2,6-dimethylphenol and 2,3,6-trimethylphenol, with poly(2,6-dimethyl-1,4-phenylene ether) being especially preferred.
These polyphenylene ether-based resins may be easily produced by the processes described in such as U.S. Pat. No. 3306874, Japanese Patent Publication No. Sho 52-17880 and Japanese Unexamined Patent Publication No. Sho 63-152628.
The polyphenylene ether-based resins used for the invention include, in addition to the polyphenylene ether-based resins mentioned above, also modified polyphenylene ether-based resins prepared by reacting the aforementioned polyphenylene ether-based resins with styrene-based monomers and/or &agr;,&bgr;-unsaturated carboxylic acids or their derivatives in the presence of or in the absence of a radical generator and in a molten state, solution state or slurry state, at a temperature of 80-350° C., where the aforementioned monomers are grafted or added at 0.01-10 wt %.
They may also be used combinations of unmodified polyphenylene ether-based resins with modified polyphenylene ether-based resins in any desired proportion.
A phosphorylated polyphenylene ether-based resin obtained by adding 9,10-dihydro-9-oxa-10-phosphaphenanthrene at 0.2-5 parts by weight to 100 parts by weight of the polyphenylene ether-based resin and melting and kneading the mixture may also be used for the invention as a polyphenylene ether-based resin with excellent color tone and flow properties.
In addition to the polyphenylene ether-based resins mentioned above, mixtures of polystyrene (for example, syndiotactic polystyrene) or high-impact polystyrene at up to 100 parts by weight to 100 parts by weight of these polyphenylene ether-based resins may also be suitably used as the (i) polyphenylene ether-based resin.
If the resulting resin composition must have durability as a heat resistant material, it is preferred to use a polyphenylene ether alone.
The polyolefin resins to be used as component (ii) for the invention are not particularly restricted, there may be mentioned polyethylene-based resins, polypropylene-based resins, polybutene-1-based resins, poly-4-methylpentene-1-based resins and the like as polyolefin resins. Polypropylene-based resins are preferred among these.
A polypropylene-based resin may be a simple propylene polymer or a copolymer with any of the monomers listed below.
As examples of preferred monomers to be used in such a copolymer there maybe mentioned linear &agr;-olefins such as ethylene, butene-1, pentene-1, hexene-1, heptene-1 and octene-1; branched &agr;-olefins such as 2-methylpropene-1,3-methylpentene-1,4-methylpentene-1,5-methylhexene-1,4-methylhexene-1 and 4,4-dimethylpentene-1; monocarboxylic acids such as acrylic acid, methacrylic acid, ethacrylic acid and crotonic acid; dicarboxylic acids such as maleic acid, fumaric acid, itaconic acid and citraconic acid, or their monoesters; acrylic acid esters or methacrylic acid esters such as methyl methacrylate, methyl acrylate and ethyl acrylate; vinyl aromatic compounds such as styrene, &agr;-methylstyrene and p-methylstyrene; acid anhydrides such as maleic anhydride, itaconic anhydride, citraconic anhydride and aconitic anhydride; &agr;,&bgr;-unsaturated nitrites such as acrylonitrile and methacrylonitrile; diene monomers such as 1,4-hexadiene, dicyclopentadiene and ethylidenenorbornane; as well as acrylamide, methacrylamide, maleimide and the like.
These copolymerizable monomers
Hattori Iwakazu
Shimakage Masashi
Takeuchi Motokazu
JSR Corporation
Mullis Jeffrey
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