Classifications

• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L71/00—Compositions of polyethers obtained by reactions forming an ether link in the main chain; Compositions of derivatives of such polymers
  • C08L71/08—Polyethers derived from hydroxy compounds or from their metallic derivatives
  • C08L71/10—Polyethers derived from hydroxy compounds or from their metallic derivatives from phenols
  • C08L71/12—Polyphenylene oxides
  • C08L71/123—Polyphenylene oxides not modified by chemical after-treatment
• • 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
  • C08K5/36—Sulfur-, selenium-, or tellurium-containing compounds
  • C08K5/41—Compounds containing sulfur bound to oxygen
  • C08K5/42—Sulfonic acids; Derivatives thereof
• • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
  • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
  • Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
  • Y10S525/00—Synthetic resins or natural rubbers -- part of the class 520 series
  • Y10S525/905—Polyphenylene oxide

Definitions

• the invention relates to a polymer mixture comprising the following constituents: A) a polyphenylene ether;
• R is an alkyl radical or aralkyl radical having 5 - 25 carbon atoms
• X is an alkali metal ion or an alka- line earth metal ion
• n 1 or 2.
• European Patent Application 0,107,835 disclo ⁇ ses a polymer mixture ' which comprises a polyphenylene ether and a polyvinyl aromatic compound to which a sulphonate is added to improve the resistance to agressive media under stress, the so-called “environmental stress crack resistance” abbreviated as ESCR.
• the kncwn mixtures have a good ESCR and a good impact strength.
• A is a block derived from a vinyl aromatic compound
• B is a block derived from a conjugated compound
• m 2 or 3
• Polymer mixtures which comprise a polypheny ⁇ lene ether, a polyvinyl aromatic compound and a block -copolymer are known per se. For this purpose reference may be made to, for example, the United States Patent Specifications 4,196,116; 4,239,673; 4,242,263;
• the improvement of the ESCR due to the preTM sence of a sulphonate and a block copolymer also occurs in polymer mixtures which comprise special polyvinyl aromatic compounds, for example, high-impact poly ⁇ styrene having a core shell structure.
• special polystyrene types lead to a high notch impact value, but polymer mixtures which have these polystyrene types generally have a low ESCR.
• the invention permits of obtaining polymer mixtures having a particularly good notch impact value in combination with an acceptab. '* e ESCR.
• the invention may also be used for polymer mixtures which, in addition to the above-mentioned constituents A, B, C and D, comprise a pigment, for example, titanium dioxide.
• a high content (of approximately 10% by weight) of titanium dioxide in a polymer mixture which comprises a polyphenylene ether and a polyvinyl aromatic compound leads to a less favourable value for the notch impact value and the ESCR.
• the polymer mixture according to the invention preferably comprises 0.5 - 5.0, even more preferably 1 - 5 parts by weight of sulphonate C and 0.5 - 10, even more preferably 2 - 5 parts by weight of block copolymer D per 100 parts by weight of A + B.
• a block copolymer is preferably used a styrene-butadiene- styrene block copolymer having a styrene content of 25 - 35% by weight, having a butadiene content of 65 - 75% by weight, in which the styrene block has a molecular weight of 5,000 to 20,000 and the block copolymer itself has a molecular weight of 50,000 to 150,000.
• the polymer mixture according to the invention may comprise 0.5 - 20 parts by weight of titanium dioxide per 100 parts by weight of A + B.
• the polymer mixture according to the invention may comprise a high-impact polystyrene based on a buta ⁇ diene rubber having a core-shell structure.
• the polymer mixture according to the invention comprises at any rate the above-mentioned constituents A, B, C and D.
• the polymer mixture may comprise further constituents.
• Polyphenylene ether are compounds which are
• Polyphenylene ethers are usually prepared by an oxidative coupling reaction - in the presence of a copper amine complex - of one or more two- or threefold substituted phenols, homopolymers and copolymers, respectively, being obtained. Copper amine complexes derived from primary, secondary and/or tertiary amine may be used.
• polyphenylene ethers examples include: poly(2,3-dimethyl-6-ethyl phenylene-l,4-ether) poly(2,3,6-trimethylphenylene-l,4-ether) poly(2-bromo-6-phenylphenylene-l,4-ether) poly(2-methyl-6-phenylphenylene-l,4-ether) poly(2-phenylphenylene-l,4-ether) poly(2-chlorophenylene-1,4-ether) poly(2-methylphenylene-1,4-ether) poly(2-chloro-6-ethylphenylene 1,4-ether) poly(2-chloro-6-bromophenylene-l,4-ether) poly(2,6-di-n-propylphenylene-l,4-ether) poly(2-methyl-6 ⁇ -isopropylphenylene-l,4-ether) poly(2-chloro-6-nethylphenylene-1,4-ether) poly(2-methyl-6-ethyl
• Copolymers for example, copolymers derived from two or more phenols as used in the preparation of the above-mentioned homopolymers, are also suitable. Furthermore graft copolymers and block copolymers of vinyl aromatic ompounds, for example polystyrene, and of a polyphenylene ether as described above are also suitable.
• the rubber-modified high-impact polyvinyl aromatic compounds are also suitable.
• polyvinyl aromatic compounds are homopoly- ers, for example, polystyrene itself, polychloro- styrene and poly-alphamethylstyrene, rubber-modified polystyrenes, for example, the commercially available high-impact polystyrene polymers and also the styrene- containing copolymers, for example, styrene-acryloni- trile copolymers, styrene-butadiene copolymers, styre- ne-acrylonitrile-butadiene terpolymers, copolymers of ethyl vinyl benzene and divinyl benzene, and the like.
• styrene-acryloni- trile copolymers for example, styrene-butadiene copolymers, styre- ne-acrylonitrile-butadiene terpolymers, copolymers of
• a so-called core-shell high-impact polystyrene may be used in the polymer mixtures according to the invention as a polyvinyl aromatic compound.
• This core- shell high-impact polystyrene is described in WO 82/02208; it is commercially available as type Polystyrene KR 2791 of BASF.
• This type of polystyrene compounds comprises a discontinuous phase consisting for the greater part of a core of polystyrene with an enveloping shell of a diene rubber diaphragm. It is also referred to as high-impact polystyrene modified with a rubber phase in the form of capsules.
• Suitable sulphonates are the following commercially available productsj C12-2O H 25-40 S ⁇ 3Na (Hostastat HS 1); c x H 2x +1 so 3 a (Atmer 190) en C ⁇ 2 H25"CgH4-S ⁇ 3N (Maranil A) .
• Suitable vinyl aromatic compounds are, for example, styrene, alpha-methylstyrene, vinyl toluene, vinyl xylene, vinylnaphtalene or mixtures of such compounds.
• Suitable conjugated diene compounds are, for example, butadiene, isoprene, 1,3-pentadiene, 2,3-dimethyl butadiene or mixtures of such compounds.
• the block copolymers may be so-called linear diblock copolymers or linear triblock copolymers. They may also be starblock copolymers.
• the block copolymers may be partly hydrogenated.
• the blocks of the block copolymer may be directly coupled together or may be coupled together via a random copolymer of a vinyl aromatic compound and a conjugated diene compound (so-called tapered block copolymers).
• a linear triblock copolymer of the type styrene-butadiene-styrene which is not hydrogenated is preferably used.
• block copolymers are known per se and are widely used in polymer mixtures which comprise a polyphenylene ether and a polyvinyl aromatic compound to improve the mechanical properties of such mixtures.
• the synergistic effect of this type of block copolymer in combination with sulphonate to improve the ESCR is new and surprising.
• the polymer mixtures according to the invention may still comprise further constituents, for example: additives to improve the flame-retarding properties, stabilizers, pigments and dyes, fillers, reinforcing fibres, antistatics, mineral oil and softeners.
• additives to improve the flame-retarding properties stabilizers, pigments and dyes, fillers, reinforcing fibres, antistatics, mineral oil and softeners.
• titanium dioxide is mentioned in particular.
• the presence of comparatively large quantities of tita ⁇ nium dioxide (of, for example, 10 parts by weight of titanium dioxide per 100 parts by weight of A + B) generally leads to a comparatively low notch impact value and a comparatively low ESCR.
• the polymer mixtures according to the invention also when they comprise comparatively much titanium dioxide, have a good notch impact value and a good ESCR.
• Example I comparative examples A, B, and C.
• polystyrene polystyrene
• PPE poly-(2,6-dimethyl- 1,4-phenylene) ether having an intrinsic viscosity of 0.48 dl/g measured in toluene at 25°C
• HIPS high- impact polystyrene
• the following usual additives were always added per 100 parts by weight of polyphenylene ether plus polystyrene: organic phosphate 10 parts by weight; titanium dioxide 12.5 parts by weight; organic phosphite 0.5 parts by weight; ZnO + ZnS 0.3 parts by weight; remaining constituents 1.05 parts by weight.
• the polymer mixture according to the com ⁇ parative example A comprised no constituents C and D; in comparative example B 2.0 parts by weight of sulpho ⁇ nate, namely Ci2-20 H 25-40 so 3 Na (Hostastat HS 1 of Hoechst) were added, in comparative example C 3.0 parts by weight of a block copolymer were added. In example I 2.0 parts by weight of the said sulphonate and 3.0 parts by weight of the same block copolymer were added.
• a block copolymer As a block copolymer was used a non-hydrogenated linear styrene-butadiene-styrene block copolymer having a styrene content of 28% by weight, a butadiene content of 72% by weight, a molecular weight of the styrene block of 11,000 and a molecular weight of the triblock copolymer of 80,000.
• compositions thus obtained are recorded in Table A below.
• the polymer mixtures were prepared by mixing the individual constituents in a Werner-Pflei- derer WP 28 extruder (adjusted temperature on an average 280 ⁇ C, flow rate 10 kg/hour, 300 r.p.m.). The resulting extrudate was chopped to pieces.
• Test bars were manufactured from the resulting pieces by injec ⁇ tion moulding. The following properties of the test bars were determined: the notch impact value according to Izod, the yield strength and the ESCR. The ESCR value was determined as follows. Test bars were manufactured (by injection moulding) according to ASTM type 1 as they are used for the determination of the tensile strength according to ASTM D 638.
• composition parts by weight
• Titanium dioxide 12.5 12.5 12.5 12.5
• polymer mixtures were prepared which comprise a special type of high-impact polystyrene instead of the usual type as used in the previous examples; in these examples a core-shell high- impact polystyrene was used as described in WO 82/02208 (BASF KR 2791).
• BASF KR 2791 BASF KR 2791
• composition parts by weight

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• Chemical Kinetics & Catalysis (AREA)
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• Organic Chemistry (AREA)
• Compositions Of Macromolecular Compounds (AREA)

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• 1984
  • 1984-10-10 NL NL8403075A patent/NL8403075A/nl not_active Application Discontinuation
• 1985
  • 1985-09-04 DE DE8585201390T patent/DE3563217D1/de not_active Expired
  • 1985-09-04 EP EP85201390A patent/EP0177989B2/en not_active Expired - Lifetime
  • 1985-10-10 US US06/786,379 patent/US4647594A/en not_active Expired - Fee Related
  • 1985-10-10 JP JP60504744A patent/JPS62500458A/ja active Granted
  • 1985-10-10 WO PCT/US1985/002001 patent/WO1986002372A1/en unknown

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