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WO2003066735A1 - Composition de resine de sulfure de polyarylene et objets moules obtenus a partir de cette composition - Google Patents

Composition de resine de sulfure de polyarylene et objets moules obtenus a partir de cette composition Download PDF

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Publication number
WO2003066735A1
WO2003066735A1 PCT/JP2003/001178 JP0301178W WO03066735A1 WO 2003066735 A1 WO2003066735 A1 WO 2003066735A1 JP 0301178 W JP0301178 W JP 0301178W WO 03066735 A1 WO03066735 A1 WO 03066735A1
Authority
WO
WIPO (PCT)
Prior art keywords
sulfide resin
polyarylene sulfide
resin composition
weight
composition according
Prior art date
Application number
PCT/JP2003/001178
Other languages
English (en)
Japanese (ja)
Inventor
Kikuo Nagatoshi
Toru Iga
Nobuyuki Kojima
Original Assignee
Idemitsu Petrochemical Co., Ltd.
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Idemitsu Petrochemical Co., Ltd. filed Critical Idemitsu Petrochemical Co., Ltd.
Publication of WO2003066735A1 publication Critical patent/WO2003066735A1/fr

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L81/00—Compositions of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing sulfur with or without nitrogen, oxygen or carbon only; Compositions of polysulfones; Compositions of derivatives of such polymers
    • C08L81/02—Polythioethers; Polythioether-ethers
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2205/00—Polymer mixtures characterised by other features
    • C08L2205/05—Polymer mixtures characterised by other features containing polymer components which can react with one another

Definitions

  • the present invention relates to a polyarylene sulfide resin composition capable of obtaining a molded article that can be used for a mirror used under severe conditions of thermal or environmental (chemical resistance, steam resistance), and using the same.
  • a polyarylene sulfide resin composition used for a vehicular lamp reflector such as a fog lamp, a headlamp and the like, and a reflector (downlight cover) of a lighting fixture and the like, and a molded article using the same.
  • thermosetting resins such as phenolic resins and unsaturated polyesters have been used as molding materials for lamp reflectors such as automotive headlamps.
  • attempts have been made to convert these thermosetting resins to thermoplastic resins due to environmental issues such as recycling.
  • the thermosetting resin composition itself has poor surface smoothness, and a resin paint is undercoated to give a mirror surface.
  • an undercoatless thermoplastic resin composition is required to simplify the process and reduce costs. ing.
  • the thermoplastic resin composition In order to achieve under-tress, the thermoplastic resin composition must have extremely high surface smoothness, as well as heat resistance and rigidity to withstand high temperatures (200-230 ° C) when the lamp is lit. It is required that high surface smoothness be obtained stably during injection molding.
  • polyallyl-lens sulfide which has high heat resistance and high fluidity, is suitable.
  • those having the above characteristics are excellent.
  • it is, of course, necessary to make the mold a mirror finish.
  • it is more easily adhered, and peeling that tends to impair the smoothness of the molded product surface is likely to occur when releasing the mold.
  • JP-A-7-188555 and JP-A-10-2327332 as a releasing agent, montanic acid and its salts, esters, polyethylene resins, etc. Is described, but there is no example.
  • Japanese Patent Application Laid-Open No. Hei 4-220364 discloses that a natural wax or the like may be added as a release agent, but there is no example.
  • Japanese Patent Application Laid-Open No. Hei 4-2722168 discloses an example in which a partially modified ester wax of montanic acid is used as a release agent.
  • the polyarylene sulfide resin composition can be used as a mirror surface because the molding temperature is usually from 300 to 350 ° C.
  • the release agent that has heat resistance that does not generate a force such as a decomposition gas and does not cause whitening of the surface due to phase separation or the like. Since the partially modified ester wax of montanic acid is inferior in heat resistance, in the case of a resin composition using the same, a large amount of volatile components is generated at the above-mentioned molding temperature, and a molded article having a mirror surface is stably molded. There was a problem.
  • polyethylene wax is an excellent mold release agent that does not generate decomposition gas and the like, and have completed the present invention.
  • an object of the present invention is to provide a polyarylene sulfide resin composition having excellent surface smoothness and mirror-like properties and capable of performing stable molding, and a molded article using the same. Disclosure of Invention ⁇
  • A 100 parts by weight of a polyarylene sulfide resin
  • B 20 to 250 parts by weight of a particulate inorganic filler
  • C whisker 0 ⁇ 50 fold
  • a polyarylene sulfide resin composition comprising 0.1 to 5 parts by weight of (D) polyethylene wax.
  • the melt viscosity of the polyarylene sulfide resin (A) is from 100 to 1,500 voids.
  • the volume average particle diameter of the particulate inorganic filler (B) is 4 / xm or less.
  • the fiber diameter of the whiskers (C) is 7 m or less.
  • the particulate inorganic filler (B) is calcium carbonate.
  • the whiskers (C) are aluminum borate whiskers.
  • the polyethylene wax (D) is an oxidized polyethylene wax.
  • a molded article obtained by molding the above-mentioned polyarylene sulfide resin composition.
  • a mirror-like body obtained by forming a metal film on a surface of the above-mentioned molded body.
  • a lamp reflector comprising the above-mentioned mirror-like body.
  • the polyarylene sulfide resin ( ⁇ ) used in the present invention preferably has a melt viscosity of 100 to 1,500 voids.
  • the melt viscosity is more preferably from 300 to 1,200 voids, and particularly preferably from 500 to 1,100 voids.
  • the melt viscosity for example, a resin temperature 3 0 0 ° C, with measurement conditions shear rate 2 0 0 se 1, can be measured by Kiyapirogurafu (manufactured by Toyo Seiki Co., Ltd.).
  • Polyarylene sulfide resin (A) is a polymer based on the structural formula [1-Ar-S-] (where Ar is an arylene group and S is iodo). Is preferably 70 mol% or more of the repeating unit represented by the following general formula (1). More preferably, it is a polymer containing at least 80 mol%. When the content of the repeating unit is less than 70 mol%, the original crystalline component, which is a characteristic of the crystalline polymer, is small, and the mechanical strength may be insufficient.
  • R 1 is an alkyl group having 6 or less carbon atoms, an alkoxy group, a phenyl group, a carboxyl group or a metal salt thereof, a nitro group, and a substituent selected from halogen atoms such as fluorine, chlorine, and bromine; m is an integer of 0 to 4. n indicates the average degree of polymerization, and is in the range of 20 to 100.
  • polyarylene sulfide resin (A) not only a homopolymer but also a copolymer can be used. Its copolymerized structural units include metaphenylene sulfide units, orthophenylene sulfide units, p, p'-diphenylene gentetone sulfide units, P, P'-diphenylene sulfone sulfide units, P, p '— Biphenylene sulfide units, p, ⁇ ' diphenylene methylene sulfide units, p, '— diphenylene cumenyl sulfide units, naphthyl sulfide units, etc.
  • the polyarylene sulfide resin (A) having a melt viscosity of 100 to 1,500 voids can be produced, for example, by the method described in JP-A-2000-186208.
  • polyarylene sulfide resin is generally known to have a molecular structure such as a linear type, a semi-linear type, or a cross-linked type, depending on the production method.
  • the polyarylene sulfide resin (A) used in the present invention is not particularly limited.
  • the molecular structure is not particularly limited.
  • the particulate inorganic filler (B) is used for expressing surface smoothness of a molded article.
  • the granular inorganic filler (B) used in the present invention has a volume average particle diameter of 4 m or less. Preferably. If the volume average particle diameter exceeds 4 m, it is difficult to ensure sufficient surface smoothness of the molded article, and when a metal film is formed on the molded article, the image clarity of the obtained mirror surface may be reduced. .
  • the volume particle size is more preferably 3.8 m or less, particularly preferably 3.5 xm or less.
  • the volume average particle diameter can be measured, for example, by a particle size distribution analyzer CIS-1 (manufactured by GALAI) using a laser-scan analysis method.
  • the blending amount of the particulate inorganic filler (B) is from 20 to 250 parts by weight per 100 parts by weight of the polyarylene sulfide resin (A). If the amount is less than 20 parts by weight, the strength of the material, particularly the rigidity, is not sufficient. On the other hand, when the amount exceeds 250 parts by weight, it is difficult to sufficiently secure the surface smoothness of the molded product, and when a metal film is formed on the molded product, the image clarity of the obtained mirror is reduced.
  • the amount of the particulate inorganic filler (B) to be blended is preferably 50 to 200 parts by weight, more preferably 60 to 150 parts by weight.
  • the type of the particulate inorganic filler (B) is not particularly limited, and any of those commonly used for polyarylene sulfide resin compositions can be used.
  • Examples of the particulate inorganic filler (B) include calcium carbonate, calcium sulfate, calcium phosphate, magnesium carbonate, magnesium oxide, magnesium phosphate, talc, myriki, silica, alumina, silica alumina, kaolin, bentonite, montmorillonite, creel , Graphite, carbon black, glass beads, titanium oxide, zirconium oxide, silicon nitride, hydrated talcite, aluminum hydroxide, and the like.
  • calcium carbonate is particularly preferred because of its stable quality and easy availability.
  • whisker (C) is used to increase the rigidity of a molded article.
  • the whiskers (C) used in the present invention preferably have a fiber diameter of 7 m or less.
  • the fiber diameter is more preferably 5 im or less, and particularly preferably 2 / x m or less.
  • the fiber diameter means the size of the minor axis of the major axis and minor axis of the fibrous material.
  • the fiber diameter can be measured, for example, by a microscope.
  • Whisker (C) is blended in a mold that requires rigidity in the molded product, and the blending amount is 0 to 50 wt.% Per 100 parts by weight of polyarylene sulfide resin (A). However, if the compounding amount exceeds 50 parts by weight, it is difficult to sufficiently secure the surface smoothness of the molded product, and when a metal film is formed on the molded product, the image clarity of the obtained mirror is reduced.
  • the compounding amount of the whiskers (C) is preferably from 0 to 40 parts by weight, and more preferably from 0 to 35 parts by weight.
  • the total amount of the particulate inorganic filler (B) and the whisker (C) is preferably not more than 250 parts by weight per 100 parts by weight of the polyarylene sulfide resin (A). If the amount exceeds 0 parts by weight, the image clarity is reduced for the same reason as described above.
  • whisker (C) is not particularly limited.
  • whiskers (C) include potassium titanate zinc, aluminum borate whiskers, calcium carbonate whiskers, calcium silicate whiskers (wollastonite), calcium silicate whiskers (zonotrite), silicon carbide whiskers, and nitriding.
  • whiskers include silicon whiskers, zinc oxide whiskers, alumina whiskers, and graphite whiskers.
  • aluminum borate whiskers are particularly preferable.
  • the polyethylene wax (D) is used as a release agent for stably forming a molded article having a mirror surface.
  • the blending amount of the polyethylene wax (D) is 0.1 to 5 parts by weight per 100 parts by weight of the polyarylene sulfide resin (A). If the compounding amount is less than 0.1, the releasability of the molded article is deteriorated, peeling marks appear on the surface of the molded article, and whitened substances are adhered, so that the surface appearance is significantly impaired. In addition, there arises a problem that the molded article adheres to the mold and the molding cycle becomes unstable. On the other hand, if it exceeds 5 parts by weight, it bleeds on the surface and impairs the surface appearance.
  • the blending amount of the polyethylene wax (D) is preferably from 0.3 to 2 parts by weight, and more preferably from 0.5 to 1.5 parts by weight.
  • the type of the polyethylene wax (D) is not particularly limited, but is preferably a polyethylene oxide wax. Oxidized polyethylene wax is a particularly excellent release agent because it has excellent heat resistance and hardly causes whitening due to phase separation.
  • the oxidized polyethylene waxes those having a large weight average molecular weight (Mw) of 50,000 to 8,000, as measured by gel permeation chromatography (GPC), particularly have volatile components.
  • the haze value in a haze test under high temperature conditions is significantly lower than 0.5%, and the weight average molecular weight of the oxidized polyethylene wax is preferably 2,0. It is preferably from 0000 to 8,000, more preferably from 4,000 to 6000. Therefore, a molded article obtained from the resin composition using the same is used as a lamp reflector. When the lamp is turned on, the lens does not fog due to volatile components even when exposed to a high temperature condition when the lamp is turned on: (230 ° C).
  • the acid preferably has an acid value of 3 or more. If the acid value is less than 3, the releasability may be insufficient.
  • the acid value of the oxidized polyethylene wax is more preferably 10 or more, and particularly preferably 15 or more.
  • the acid value means mg of potassium hydroxide required to neutralize 1 g of wax.
  • the polyarylene sulfide resin composition of the present invention contains a silane coupling agent, an antioxidant, a heat stabilizer, a lubricant, a plasticizer, a conductivity-imparting agent, if necessary, as long as the effects of the present invention are not impaired.
  • Various additives such as colorants and pigments may be further compounded.
  • the method for producing the polyarylene sulfide resin composition of the present invention is not particularly limited. Examples of the method include melt kneading using a ripon tumbler, a Henschel mixer, a Banbury mixer, a drum tumbler, a single screw extruder, or the like. In this case, an appropriate kneading temperature is usually from 300 to 350 ° C. 3. Molded product
  • the polyarylene sulfide resin composition of the present invention can be molded by a molding method such as injection molding and injection compression molding.
  • molded products obtained by injection molding are excellent in surface smoothness, and even when exposed to high temperatures for a long time (for example, 230 or 24 hours), the surface becomes white and the surface such as Z or flow mark becomes good. Haze is extremely small due to little change in appearance and small amount of volatile components.
  • such a molded article has excellent releasability at the time of injection molding, so that there is no peeling mark on the surface. Therefore, molding can be performed stably for a long time in a state of high mirror finish.
  • Such a molded article can be made into a mirror-like body by forming a metal film such as aluminum on the surface, for example, a lamp reflector for automobiles such as fog lamps and headlamps, and a reflector (such as a lighting fixture). Light cover) can be used.
  • a metal film such as aluminum on the surface
  • a lamp reflector for automobiles such as fog lamps and headlamps
  • a reflector such as a lighting fixture.
  • Light cover can be used.
  • the obtained pellets were formed into a flat plate (80 ⁇ 80 ⁇ 2 mm) using a mirror-finished flat plate (80 ⁇ 80 ⁇ 2 mm) attached to a 50-ton injection molding machine (manufactured by JSW, J50E-P).
  • the unit of the amount of each component constituting the polyarylene sulfide resin composition is part by weight, the melt viscosity of PPS, the volume average particle size of calcium carbonate, and aluminum borate whiskers.
  • the weight average molecular weight (Mw) of the fiber warp and the oxidized polyethylene wax was measured by the measurement method described above.
  • ⁇ The mold release is smooth and there is no abnormality such as peeling marks on the surface.
  • Aluminum was vacuum-deposited (thickness: about 100 nm) on the surface of the flat molded product, and measured by an image clarity tester (manufactured by Suga Test Instruments Co., Ltd.).
  • the measurement principle is that the reflected image of the light source is diffused due to the reflection performance of the reflector (an image larger than the specular reflection image), so the light received through the optical slit (created with a fixed grid pattern) is observed.
  • the test piece is set so that the incident angle of the light source is 45 degrees, and the optical slit (optical comb width: 1.0 mm) is set perpendicular to the direction of the reflection angle of 45 degrees.
  • the receiver is set ahead, an image of the light source is projected on the optical slit, the slit is moved in the setting direction, and the minimum amount of light detected by the receiver via the slit is defined as the maximum reflectance M.
  • the image clarity (C value) is expressed as (M ⁇ m) Z (M + m) X100 (%), with the maximum light quantity as the minimum reflectance m.
  • PP S (1) Polyphenylene sulfide resin (produced by DIP Corp., K-1, melt viscosity 390 boise)
  • Calcium carbonate (1) Caltex 5 (manufactured by Maruo Calcium Co., Ltd.), volume average particle size 1.0 ⁇
  • Calcium carbonate (2) SL 2200 (manufactured by Takehara Chemical Industry Co., Ltd.), volume average particle size 3.5 urn
  • Oxidized polyethylene wax (1) Licowax PED 191 (made by Clariant Japan)
  • PP S (1) Polyphenylene sulfide resin (manufactured by DIC Corporation, K-1; melt viscosity 390 boise)
  • Calcium carbonate (2) SL 2200 (manufactured by Takehara Chemical Industry Co., Ltd.), volume average particle
  • Licowax PED 191 (Clarian Toji)
  • P P S (2) Polyphenylene sulfide resin (LDN-1G, melt viscosity 500 boise, manufactured by DIC Corporation)
  • Calcium carbonate (2) SL 2200 (manufactured by Takehara Chemical Industry Co., Ltd.), volume average particle diameter 3.5 m
  • Aluminum borate whiskers Albolex YS 2B (Shikoku Chemicals Co., Ltd. Fiber diameter 0.5-1.0 m, L / D: 10-
  • PP S (2) Polyphenylene sulfide resin (LN-1G, melt viscosity 500 boise, manufactured by DIC Corporation)
  • PP S (3) Polyphenylene sulfide resin (manufactured by DIP Corp., LN_2G, melt viscosity 1,050 boise)
  • PPS (4) Polyphenylene sulfide resin (Tosoichi # 160, melt viscosity 1,800 Boyes)
  • Calcium carbonate (2) SL 2200 (manufactured by Takehara Chemical Industry Co., Ltd.), volume average particle size 3.5 urn
  • Oxidized polyethylene wax (1) Licowax PED 191 (made by Clariant Japan)
  • a polyarylene sulfide resin composition having excellent surface smoothness and specularity and capable of performing stable molding, and a molded article using the same.

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  • Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Manufacture Of Macromolecular Shaped Articles (AREA)
  • Non-Portable Lighting Devices Or Systems Thereof (AREA)

Abstract

La présente invention concerne une composition de résine de sulfure de polyarylène qui comprend (A) 100 parts par poids d'une résine de sulfure de polyarylène, (B) de 20 à 250 parts par poids d'une charge particulaire inorganique, (C) de 0 à 50 parts par poids de trichite et (D) de o,1 à 5 parts par poids d'une paraffine polyarylène. Cette invention concerne aussi un objet spéculaire comprenant un moulage de cette composition de résine de sulfure de polyarylène et un film métallique déposé sur une surface de ce moulage utilisable comme réflecteur de lampe, etc..
PCT/JP2003/001178 2002-02-06 2003-02-05 Composition de resine de sulfure de polyarylene et objets moules obtenus a partir de cette composition WO2003066735A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2002-29492 2002-02-06
JP2002029492A JP2003226810A (ja) 2002-02-06 2002-02-06 ポリアリーレンスルフィド樹脂組成物及びそれを用いた成形体

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108603031A (zh) * 2016-03-09 2018-09-28 英驰株式会社 用于灯具反射器的具有优异的表面光滑度和金属附着力的树脂组合物

Families Citing this family (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
MX337377B (es) 2012-03-23 2016-03-01 Dainippon Ink & Chemicals Composicion de resina de sulfuro de poliarileno y cuerpo moldeado.
WO2013168313A1 (fr) * 2012-05-11 2013-11-14 ポリプラスチックス株式会社 Composition de résine destinée à un composant réfléchissant la lumière
KR20150023780A (ko) * 2012-06-26 2015-03-05 포리프라스틱 가부시키가이샤 광반사 부품 및 그 제조방법
EP4450551A3 (fr) * 2019-11-26 2025-01-15 DIC Corporation Composition de résine de sulfure de polyarylène, article moulé, produit stratifié et son procédé de production

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS5447752A (en) * 1977-09-19 1979-04-14 Phillips Petroleum Co Method of improving processability of arylenesulfide polymer composition
JP2000186208A (ja) * 1998-12-21 2000-07-04 Idemitsu Petrochem Co Ltd ポリアリーレンスルフィド樹脂組成物及びそれからなる鏡面体・ランプリフレクター
JP2001288363A (ja) * 2000-02-01 2001-10-16 Polyplastics Co 耐トラッキング性が良好な強化ポリアリーレンサルファイド樹脂組成物
WO2002000794A1 (fr) * 2000-06-29 2002-01-03 Idemitsu Petrochemical Co., Ltd. Composition de resine de sulfure de polyarylene

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS5447752A (en) * 1977-09-19 1979-04-14 Phillips Petroleum Co Method of improving processability of arylenesulfide polymer composition
JP2000186208A (ja) * 1998-12-21 2000-07-04 Idemitsu Petrochem Co Ltd ポリアリーレンスルフィド樹脂組成物及びそれからなる鏡面体・ランプリフレクター
JP2001288363A (ja) * 2000-02-01 2001-10-16 Polyplastics Co 耐トラッキング性が良好な強化ポリアリーレンサルファイド樹脂組成物
WO2002000794A1 (fr) * 2000-06-29 2002-01-03 Idemitsu Petrochemical Co., Ltd. Composition de resine de sulfure de polyarylene

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108603031A (zh) * 2016-03-09 2018-09-28 英驰株式会社 用于灯具反射器的具有优异的表面光滑度和金属附着力的树脂组合物
EP3428234A4 (fr) * 2016-03-09 2019-10-02 Initz Co., Ltd. Composition de résine pour un réflecteur de lampe présentant un excellent lissé de surface et un excellent dépôt de métal
CN108603031B (zh) * 2016-03-09 2020-09-22 Sk化学公司 用于灯具反射器的具有优异的表面光滑度和金属附着力的树脂组合物
TWI713700B (zh) 2016-03-09 2020-12-21 南韓商Ｓｋ化學公司 具有良好表面粗糙度及金屬沈積之燈反射器用樹脂組成物

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