WO2020004997A1 - Composition de résine thermoplastique et produit moulé formé à partir de celle-ci - Google Patents

Composition de résine thermoplastique et produit moulé formé à partir de celle-ci Download PDF

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Publication number
WO2020004997A1
WO2020004997A1 PCT/KR2019/007854 KR2019007854W WO2020004997A1 WO 2020004997 A1 WO2020004997 A1 WO 2020004997A1 KR 2019007854 W KR2019007854 W KR 2019007854W WO 2020004997 A1 WO2020004997 A1 WO 2020004997A1
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WO
WIPO (PCT)
Prior art keywords
resin composition
thermoplastic resin
weight
polyamide
astm
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PCT/KR2019/007854
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English (en)
Korean (ko)
Inventor
반균하
최원영
진영섭
Original Assignee
롯데첨단소재(주)
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Publication of WO2020004997A1 publication Critical patent/WO2020004997A1/fr

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F212/00—Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by an aromatic carbocyclic ring
    • C08F212/02—Monomers containing only one unsaturated aliphatic radical
    • C08F212/04—Monomers containing only one unsaturated aliphatic radical containing one ring
    • C08F212/06—Hydrocarbons
    • C08F212/08—Styrene
    • 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
    • C08K3/01—Use of inorganic substances as compounding ingredients characterized by their specific function
    • C08K3/013—Fillers, pigments or reinforcing additives
    • 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
    • C08K3/34—Silicon-containing compounds
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L25/00—Compositions of, homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by an aromatic carbocyclic ring; Compositions of derivatives of such polymers
    • C08L25/02—Homopolymers or copolymers of hydrocarbons
    • C08L25/04—Homopolymers or copolymers of styrene
    • C08L25/08—Copolymers of styrene
    • 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
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L77/00—Compositions of polyamides obtained by reactions forming a carboxylic amide link in the main chain; Compositions of derivatives of such polymers
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F2500/00—Characteristics or properties of obtained polyolefins; Use thereof
    • C08F2500/12—Melt flow index or melt flow ratio

Definitions

  • the present invention relates to a thermoplastic resin composition and a molded article formed therefrom. More specifically, the present invention relates to a thermoplastic resin composition excellent in dimensional stability, appearance characteristics, impact resistance, rigidity, heat resistance, and the like and molded articles formed therefrom.
  • Plastic materials are excellent in light weight, design freedom, molding processability, etc., and are widely applied to fields requiring various functions and performances such as industrial materials such as household goods, automobiles, electrical, electronics, and industrial fields.
  • polyphenylene ether resin has excellent electrical and mechanical properties, has a high heat deformation temperature, and is used in a wide range of fields as an engineering plastic material.
  • the resin composition containing polyphenylene ether resin and polyamide resin can express physical properties, such as heat resistance, impact resistance, and chemical resistance, in balance, and is utilized for automobile exterior parts.
  • polyphenylene ether resins and polyamide resin blends may cause dimensional changes due to temperature or humidity changes, and an inorganic filler is used to reduce them.
  • an inorganic filler is used to reduce them.
  • a problem may occur in that the appearance characteristics, etc., are greatly lowered, and mechanical properties, etc., are lowered due to the lowering of the compatibility of the resin composition.
  • thermoplastic resin composition having excellent dimensional stability, appearance characteristics, impact resistance, rigidity, heat resistance, and the like without these problems.
  • Patent Publication No. 2014-0086736 discloses in, for example, Patent Publication No. 2014-0086736.
  • An object of the present invention is to provide a thermoplastic resin composition excellent in dimensional stability, appearance characteristics, impact resistance, rigidity, heat resistance and the like.
  • Another object of the present invention is to provide a molded article formed from the thermoplastic resin composition.
  • thermoplastic resin composition comprises about 100 parts by weight of a base resin comprising about 10 to about 45 weight percent of a polyphenylene ether resin, and about 55 to about 90 weight percent of an aliphatic polyamide resin; About 10 to about 40 parts by weight of an inorganic filler; And about 2 to about 10 parts by weight of a styrene-ethylene / butylene-styrene copolymer, wherein the weight ratio of the inorganic filler and the styrene-ethylene / butylene-styrene copolymer is about 3: 1 to about 8: 1 It is characterized by that.
  • the polyphenylene ether resin may include a repeating unit represented by Formula 1 below:
  • R 1 , R 2 , R 3 and R 4 are each independently a hydrogen atom, a halogen atom, an alkyl group having 1 to 6 carbon atoms or an aryl group having 6 to 12 carbon atoms.
  • the aliphatic polyamide resin may include at least one of polyamide 6, polyamide 11, polyamide 12, polyamide 4.6, polyamide 6.6 and polyamide 6.10.
  • the inorganic filler may be a plate-shaped inorganic filler.
  • the inorganic filler may include one or more of talc, chlorite and mica.
  • the styrene-ethylene / butylene-styrene copolymer has a melt flow index (MI) measured at 200 °C, 5 kgf conditions in accordance with ASTM D1238 10 to about 50 g / 10 minutes.
  • the thermoplastic resin composition may have a linear expansion coefficient of about 30 to about 100 ⁇ m / m ⁇ °C measured on a 6.4 mm thick specimen at 90 °C according to ASTM D696.
  • thermoplastic resin composition may have a gloss difference of about 3 GU or less calculated according to Equation 1 below:
  • G 0 is the gate part glossiness of 100 mm ⁇ 100 mm ⁇ 3.2 mm size injection molded specimen measured at 60 ° angle according to ASTM D523
  • G 1 is at 60 ° angle according to ASTM D523 Measured glossiness of the tip (as opposed to the gate) of the 100 mm ⁇ 100 mm ⁇ 3.2 mm size injection molded specimens measured.
  • thermoplastic resin composition may have a notched Izod impact strength of about 1/8 "thick specimen, measured in accordance with ASTM D256, from about 4 to about 20 kgf ⁇ cm / cm.
  • thermoplastic resin composition has a tensile strength of about 600 to about 800 kgf / cm 2 measured at a rate of 5 mm / min using a 3.2 mm thick specimen in accordance with ASTM D638 Can be.
  • the thermoplastic resin composition has a heat deflection temperature (HDT) of about 210 to about 240 measured at a load of 18.56 kgf / cm 2 , the temperature increase rate of 120 °C / hr in accordance with ASTM D648 May be ° C.
  • HDT heat deflection temperature
  • the molded article is formed from the thermoplastic resin composition according to any one of 1 to 11.
  • the present invention has the effect of providing the thermoplastic resin composition excellent in dimensional stability, appearance properties, impact resistance, rigidity, heat resistance and the like and a molded article formed therefrom.
  • thermoplastic resin composition according to the present invention comprises (A) a polyphenylene ether resin; (B) aliphatic polyamide resins; (C) inorganic fillers; And (D) styrene-ethylene / butylene-styrene copolymer.
  • Polyphenylene ether resin according to an embodiment of the present invention is to improve the heat resistance, hydrolysis resistance, etc. of the thermoplastic resin composition, and to reduce the hygroscopic deformation, polyphenylene ether resin used in ordinary thermoplastic resin compositions Can be used.
  • a polyphenylene ether containing a repeating unit represented by the following formula (1) may be used.
  • R 1 , R 2 , R 3 and R 4 are each independently a hydrogen atom, a halogen atom, an alkyl group having 1 to 6 carbon atoms or an aryl group having 6 to 12 carbon atoms.
  • the polyphenylene ether resin may be poly (1,4-phenylene) ether, poly (2,6-dimethyl-1,4-phenylene) ether, poly (2,6-diethyl-1 , 4-phenylene) ether, poly (2,6-dipropyl-1,4-phenylene) ether, poly (2-methyl-6-ethyl-1,4-phenylene) ether, poly (2-methyl -6-propyl-1,4-phenylene) ether, poly (2-ethyl-6-propyl-1,4-phenylene) ether, poly (2,6-diphenyl-1,4-phenylene) ether , Copolymers of poly (2,6-dimethyl-1,4-phenylene) ether and poly (2,3,6-trimethyl-1,4-phenylene) ether, poly (2,6-dimethyl-1, And copolymers of 4-phenylene) ether and poly (2,3,5-triethyl-1,4-phenylene)
  • the polyphenylene ether resin may have a weight average molecular weight of about 10,000 to about 50,000 g / mol, for example, about 20,000 to about 40,000 g / mol, as measured by gel permeation chromatography (GPC).
  • the thermoplastic resin composition may be excellent in heat resistance, mechanical properties, processability and the like.
  • the polyphenylene ether resin is about 10 to about 45 weight percent of 100 weight percent of a basic resin (A + B) comprising a polyphenylene ether resin (A) and an aliphatic polyamide resin (B), For example, about 20 to about 35 weight percent.
  • a basic resin A + B
  • the content of the polyphenylene ether resin is less than about 10% by weight, heat resistance, dimensional stability, etc. of the thermoplastic resin composition may be lowered.
  • the content of the polyphenylene ether resin is greater than about 40% by weight, the molding processability (fluidity) of the thermoplastic resin composition may be reduced. And stiffness may be lowered.
  • the aliphatic polyamide resin according to one embodiment of the present invention can improve molding processability (fluidity), rigidity, and the like of the thermoplastic resin composition, and may use an aliphatic polyamide resin used in a conventional thermoplastic resin composition.
  • the aliphatic polyamide resin can be polyamide 6, polyamide 11, polyamide 12, polyamide 4.6, polyamide 6.6, polyamide 6.10, combinations thereof, and the like.
  • polyamide 6, polyamide 6.6 and the like can be used.
  • the aliphatic polyamide resin may have a melting temperature (Tm) measured by differential scanning calorimetry (DSC) of about 255 to about 275 °C, for example about 260 to about 270 °C. Molding processability, heat resistance and the like of the thermoplastic resin composition may be excellent in the above range.
  • Tm melting temperature measured by differential scanning calorimetry
  • the aliphatic polyamide resin is dissolved in concentrated sulfuric acid (96%) solution at a concentration of 0.5 g / dL, and has an intrinsic viscosity (IV) of about 2 measured at 25 ° C. using an Ubbelodhde viscometer.
  • IV intrinsic viscosity
  • the molding processability (fluidity), impact resistance, rigidity, and the like of the thermoplastic resin composition may be excellent.
  • the aliphatic polyamide resin is from about 55 to about 90 weight percent, in 100 weight percent of base resin (A + B) comprising polyphenylene ether resin (A) and aliphatic polyamide resin (B) For example, about 65 to about 80 weight percent.
  • base resin A + B
  • polyphenylene ether resin A
  • aliphatic polyamide resin B
  • the content of the aliphatic polyamide resin is less than about 55% by weight, the molding processability (flowability), rigidity, etc. of the thermoplastic resin composition may be lowered.
  • the content of the aliphatic polyamide resin is greater than about 90% by weight, the heat resistance and dimensions of the thermoplastic resin composition may be reduced. There is a possibility that the stability or the like is lowered.
  • the inorganic filler according to one embodiment of the present invention can improve the dimensional stability, rigidity, and the like of the thermoplastic resin composition, and reduce the hygroscopic deformation, and may use a conventional plate-shaped inorganic filler.
  • the inorganic filler may be talc, chlorite, mica, a combination thereof, or the like.
  • conventional plate-shaped talc can be used.
  • the average particle size of the plate-shaped inorganic filler may be about 2 to about 10 ⁇ m, for example about 3 to about 7 ⁇ m.
  • the thermoplastic resin composition may have excellent dimensional stability, rigidity, fluidity, appearance characteristics, and the like.
  • the inorganic filler may be included in an amount of about 10 to about 40 parts by weight, for example about 15 to about 30 parts by weight, based on about 100 parts by weight of the base resin.
  • the content of the inorganic filler is less than about 10 parts by weight based on about 100 parts by weight of the base resin, the dimensional stability, rigidity, and the like of the thermoplastic resin composition are lowered, there is a risk of hygroscopic deformation, and may exceed about 40 parts by weight. In the case, there exists a possibility that the external appearance characteristic, impact resistance, etc. of a thermoplastic resin composition may fall.
  • Styrene-ethylene / butylene-styrene copolymer according to one embodiment of the present invention is applied with an inorganic filler, impact resistance, dimensional stability, rigidity without deterioration in appearance characteristics of the thermoplastic resin composition (molded article), etc.
  • SEBS Styrene-ethylene / butylene-styrene copolymer
  • the styrene ethylene / butylene styrene copolymer applied to a normal thermoplastic resin composition can be used.
  • the styrene-ethylene / butylene-styrene copolymer has a melt-flow index (MI) of about 10 to about 50 g /, measured at 200 ° C. and 5 kgf, based on ASTM D1238. 10 minutes, for example about 12 to about 48 g / 10 minutes.
  • MI melt-flow index
  • the thermoplastic resin composition may have excellent impact resistance, dimensional stability, rigidity, flowability, appearance characteristics, and the like.
  • the styrene-ethylene / butylene-styrene copolymer may be included in about 2 to about 10 parts by weight, for example about 3 to about 8 parts by weight, based on about 100 parts by weight of the base resin.
  • the content of the styrene-ethylene / butylene-styrene copolymer is less than about 2 parts by weight based on about 100 parts by weight of the base resin, there is a fear that the appearance characteristics, impact resistance, etc. of the thermoplastic resin composition may be lowered, and about 10 parts by weight. When it exceeds a part, there exists a possibility that the external appearance characteristic, heat resistance, etc. of a thermoplastic resin composition may fall.
  • the weight ratio (C: D) of the inorganic filler (C) and the styrene-ethylene / butylene-styrene copolymer (D) is about 3: 1 to about 8: 1, for example about 3.3: 1 To about 7.8: 1.
  • the weight ratio is less than about 3: 1, the dimensional stability of the thermoplastic resin composition is lowered, and there is a possibility that hygroscopic deformation occurs, and when it is greater than about 8: 1, the appearance characteristics, impact resistance, heat resistance, and the like of the thermoplastic resin composition There is a risk of deterioration.
  • the thermoplastic resin composition according to one embodiment of the present invention may further include an additive included in a conventional thermoplastic resin composition.
  • the additives may include, but are not limited to, a compatibilizer, a flame retardant, an antioxidant, an antidrip agent, a lubricant, a mold release agent, a nucleating agent, a stabilizer, a pigment, a dye, a mixture thereof, and the like.
  • the content may be about 0.001 to about 40 parts by weight, for example about 0.1 to about 10 parts by weight, based on about 100 parts by weight of the base resin.
  • thermoplastic resin composition according to one embodiment of the present invention may be in the form of pellets mixed with the components and melt-extruded at about 250 to about 320 ° C, for example, about 280 to about 300 ° C, using a conventional twin screw extruder. Can be.
  • the thermoplastic resin composition has a linear expansion coefficient of about 30 to about 100 ⁇ m / m ⁇ ° C., for example about 40 to about 90 ⁇ m / m, measured on a 6.4 mm thick specimen at 90 ° C. according to ASTM D696. May be ° C.
  • the difference in glossiness calculated according to Equation 1 may be about 3 GU (gloss units) or less, for example, about 0.5 to about 2.5 GU.
  • G 0 is the gate part glossiness of 100 mm ⁇ 100 mm ⁇ 3.2 mm size injection molded specimen measured at 60 ° angle according to ASTM D523
  • G 1 is at 60 ° angle according to ASTM D523 Measured glossiness of the tip (as opposed to the gate) of the 100 mm ⁇ 100 mm ⁇ 3.2 mm size injection molded specimens measured.
  • the thermoplastic resin composition has a notched Izod impact strength of about 1/8 "thick specimen, measured in accordance with ASTM D256, from about 4 to about 20 kgfcm / cm, for example from about 4.5 to about 10 kgf. may be cm / cm.
  • the thermoplastic resin composition has a tensile strength of about 600 to about 800 kgf / cm 2 , for example from about 610 to 5 mm / min, using a 3.2 mm thick specimen in accordance with ASTM D638. About 750 kgf / cm 2 .
  • the thermoplastic resin composition has a heat deflection temperature (HDT) of about 210 to about 240 ° C., for example, about 18.56 kgf / cm 2 , a heating rate of 120 ° C./hr, based on ASTM D648. 210 to about 230 ° C.
  • HDT heat deflection temperature
  • the molded article according to the present invention is formed from the thermoplastic resin composition.
  • the thermoplastic resin composition may be prepared in a pellet form, and the prepared pellet may be manufactured into various molded products (products) through various molding methods such as injection molding, extrusion molding, vacuum molding, and casting molding. Such molding methods are well known by those skilled in the art. Since the molded article is excellent in dimensional stability, appearance characteristics, impact resistance, rigidity, heat resistance, balance of physical properties, etc., it is useful as automotive interior / exterior materials, interior / exterior materials of electrical / electronic products, building exterior materials and the like.
  • Polyamide 6.6 (manufacturer: Ascend Performance Materials, product name: Vydyne® 50BW, melting temperature (Tm): 260 ° C) was used.
  • each of the constituents is added in an amount as shown in Table 1 below, wherein the polyphenylene ether resin is side fed with styrene-ethylene / butylene-styrene copolymer or maleic anhydride-modified ethylene-octene copolymer.
  • the physical properties of the prepared specimens were evaluated by the following method, and the results are shown in Table 1 below.
  • G 0 is the gate part glossiness of 100 mm ⁇ 100 mm ⁇ 3.2 mm size injection molded specimen measured at 60 ° angle according to ASTM D523
  • G 1 is at 60 ° angle according to ASTM D523 Measured glossiness of the tip (as opposed to the gate) of the 100 mm ⁇ 100 mm ⁇ 3.2 mm size injection molded specimens measured.
  • Notched Izod impact strength (unit: kgf ⁇ cm / cm): Notched Izod impact strength of a 1/8 "thick specimen was measured according to ASTM D256.
  • Heat distortion temperature (HDT, unit: degreeC): Based on ASTMD648, the heat distortion temperature was measured on the conditions of 18.56 kgf / cm ⁇ 2> of loads and the temperature increase rate of 120 degreeC / hr.
  • thermoplastic resin composition of the present invention is excellent in all of dimensional stability, appearance characteristics, impact resistance, rigidity, heat resistance and the like.
  • Comparative Example 1 in which the content of the styrene-ethylene / butylene-styrene copolymer is less than the range of the present invention, it can be seen that impact resistance, appearance characteristics (gloss uniformity), etc. of the thermoplastic resin composition are reduced, and styrene-ethylene
  • Comparative Example 2 in which the content of the / butylene-styrene copolymer is greater than the range of the present invention, it can be seen that the rigidity, heat resistance, and the like of the thermoplastic resin composition are reduced.

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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)

Abstract

La présente invention concerne une composition de résine thermoplastique comprenant : environ 100 parties en poids de résines de base comprenant environ 10 à 45 % en poids d'une résine de poly(phénylène éther) et environ 55 à 90 % en poids d'une résine de polyamide aliphatique ; environ 10 à 40 parties en poids d'une charge inorganique ; et environ 2 à 10 parties en poids d'un copolymère styrène-éthylène/butylène-styrène, le rapport pondéral de la charge inorganique au copolymère styrène-éthylène/butylène-styrène étant d'environ 3:1 à 8:1. La composition de résine thermoplastique est excellente en matière de stabilité dimensionnelle, de propriétés extérieures, de résistance aux chocs, de rigidité, de résistance à la chaleur etc.
PCT/KR2019/007854 2018-06-29 2019-06-28 Composition de résine thermoplastique et produit moulé formé à partir de celle-ci WO2020004997A1 (fr)

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KR10-2018-0075313 2018-06-29
KR1020180075313A KR102245330B1 (ko) 2018-06-29 2018-06-29 열가소성 수지 조성물 및 이로부터 형성된 성형품

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Publication number Priority date Publication date Assignee Title
KR102700764B1 (ko) * 2021-06-30 2024-08-29 롯데케미칼 주식회사 열가소성 수지 조성물 및 이로부터 형성된 성형품

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5475049A (en) * 1992-11-09 1995-12-12 General Electric Company Resin composition
KR20130113118A (ko) * 2012-04-05 2013-10-15 한국화학연구원 전기전도성 향상 수지 조성물
KR20140086736A (ko) * 2012-12-28 2014-07-08 제일모직주식회사 열가소성 수지 조성물 및 이를 포함한 성형품
KR20140087907A (ko) * 2012-12-31 2014-07-09 제일모직주식회사 열가소성 수지 조성물 및 이를 포함한 성형품
KR20170080172A (ko) * 2015-12-31 2017-07-10 롯데첨단소재(주) 폴리아미드/폴리페닐렌 에테르 수지 조성물 및 이로부터 제조된 자동차용 성형품

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5475049A (en) * 1992-11-09 1995-12-12 General Electric Company Resin composition
KR20130113118A (ko) * 2012-04-05 2013-10-15 한국화학연구원 전기전도성 향상 수지 조성물
KR20140086736A (ko) * 2012-12-28 2014-07-08 제일모직주식회사 열가소성 수지 조성물 및 이를 포함한 성형품
KR20140087907A (ko) * 2012-12-31 2014-07-09 제일모직주식회사 열가소성 수지 조성물 및 이를 포함한 성형품
KR20170080172A (ko) * 2015-12-31 2017-07-10 롯데첨단소재(주) 폴리아미드/폴리페닐렌 에테르 수지 조성물 및 이로부터 제조된 자동차용 성형품

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