WO2012157841A1 - Composition de polymère possédant une bonne conductivité thermique supérieure et procédé de préparation de ladite composition - Google Patents

Composition de polymère possédant une bonne conductivité thermique supérieure et procédé de préparation de ladite composition Download PDF

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Publication number
WO2012157841A1
WO2012157841A1 PCT/KR2012/001662 KR2012001662W WO2012157841A1 WO 2012157841 A1 WO2012157841 A1 WO 2012157841A1 KR 2012001662 W KR2012001662 W KR 2012001662W WO 2012157841 A1 WO2012157841 A1 WO 2012157841A1
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WIPO (PCT)
Prior art keywords
volume
polymer composition
thermal conductivity
filler
present
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English (en)
Korean (ko)
Inventor
이성구
유영재
원종찬
김해운
전병국
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Korea Research Institute of Chemical Technology
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Korea Research Institute of Chemical Technology
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    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
    • C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L69/00—Compositions of polycarbonates; Compositions of derivatives of polycarbonates
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
    • 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
    • C08K3/02—Elements
    • C08K3/04—Carbon
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2323/00—Characterised by the use of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Derivatives of such polymers
    • C08J2323/02—Characterised by the use of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Derivatives of such polymers not modified by chemical after treatment
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2369/00—Characterised by the use of polycarbonates; Derivatives of polycarbonates

Definitions

  • the present invention relates to a polymer composition excellent in thermal conductivity, a molded article produced therefrom, and a method for producing the same.
  • metal is most often used as a material such as a heat sink of an electronic device having an invented component. This is because of the high thermal conductivity of metals. Metal diffuses heat faster than other materials, protecting electronic components that are sensitive to heat. In addition, the metal has a high mechanical strength has the advantage of being suitable as a heat radiation material.
  • these metals are disadvantageous due to their high density, which is difficult to reduce in weight, poor in workability, and high in manufacturing cost.
  • thermally conductive polymer compositions that can replace metals.
  • the research on the thermally conductive polymer composition has been mainly conducted through the composite technology of the polymer and the thermally conductive filler, and until now, the breakthrough technology for improving the thermal conductivity of the polymer material is insufficient except the composite technology of the polymer and the thermally conductive filler.
  • the polymer material has a thermal conductivity of 0.1 to 0.5 W / (m ⁇ K) and is a thermal resistance, and in the case of a composite material containing a large amount of thermally conductive fillers, the thermal conductivity of about 10 W / (m ⁇ K) is also common.
  • the composite material having such a thermal conductivity includes a very high content of thermally conductive fillers, workability decreases with rapid increase in viscosity, and mechanical properties are greatly reduced.
  • the composite material having such a thermal conductivity includes a very high content of thermally conductive fillers, workability decreases with rapid increase in viscosity, and mechanical properties are greatly reduced.
  • the problem that the local high temperature which arises in an electronic device causes malfunction or ignition of an electronic device is largely highlighted. Therefore, the demand for polymer materials having high thermal conductivity and excellent workability is increasing.
  • thermally conductive polymer compositions are not sufficiently high in thermal conductivity, and in the case of a material that satisfies thermal conductivity, they are poor in workability, and molding is not possible through existing extrusion or injection processes. Not enough to
  • Korean Patent Publication No. 10-2010-0075227 relates to a polymer resin composition having excellent thermal conductivity, and uses a large amount of filler by effectively constructing a network between fillers using fillers of different shapes and sizes.
  • the polymer resin composition which is excellent in thermal conductivity and excellent in mechanical strength is described.
  • the invention is an invention for improving the thermal conductivity in a way to improve the contact area between the pillars.
  • 6,899,160 also relates to a thermally conductive material having improved thermal conductivity by using two or more fillers, and the contact between the fillers by using two different thermally conductive fillers similar to the Korean Patent Publication.
  • the thermal conductivity is improved by improving the rate and reducing the thickness of the matrix.
  • Japanese Laid-Open Patent Publication No. 2009-292889 is an invention in which a filler is sufficiently included to improve thermal conductivity, and further includes polyamide fibers to prevent deterioration of mechanical properties.
  • the thermal conductivity of the composite is 10 W / (m ⁇ K) or less, so that the thermal conductivity of the composite is low so that its use is limited. Accordingly, the inventors of the present invention, while studying to improve the thermal conductivity of the polymer composition in a completely different method until now, by mixing two different polymers and fillers, and controlling their morphology (morphology) to improve the thermal conductivity of the polymer composition The present invention was improved.
  • An object of the present invention is to provide a polymer composition having excellent thermal conductivity and excellent mechanical strength, and a molded article prepared therefrom. Another object of the present invention to provide a method for producing the polymer composition and molded article.
  • the present invention is 10 to 80% by volume of a polycarbonate resin; 10 to 80% by volume polyolefin resin; And 5 to 80% by volume of thermally and electrically conductive fillers and molded articles prepared therefrom, 10 to 80% by volume of polycarbonate resins, 10 to 80% by volume of polyolefinic resins, and 5 Mixing from about 80% by volume of the thermally conductive filler; And it provides a method for producing a polymer composition comprising the step of extruding the mixture.
  • the thermal conductivity is greatly improved by effectively forming a network between the fillers by controlling the morphology of two or more polymers in the composition while using one filler. Accordingly, the molded article prepared from the polymer composition according to the present invention may be usefully applied to parts such as heat sinks of electronic devices.
  • FIG. 1 is a schematic diagram showing an enlarged conventional polymer composition including a filler
  • Figure 2 is an enlarged schematic diagram showing the polymer composition according to an embodiment of the present invention.
  • the present invention solves the problem in a method different from the known inventions in improving the thermal conductivity of the polymer composition.
  • the known inventions include: 1) a method that includes a filler sufficiently, but further includes means for preventing the mechanical properties from deteriorating; and 2) a method of improving the contact ratio between the fillers, including fillers of different types or types.
  • the thermal conductivity is improved
  • the present invention controls the morphology to form two phases by mixing two kinds of non-mixing polymers, but one of the two phases is to have a high affinity for the filler, the filler Improves thermal conductivity by effectively organizing the network of fillers in such a way that is present in a single phase.
  • the present invention is a.
  • Polycarbonate-based resins and polyolefin-based resins do not have compatibility with each other, and when they are mixed, they form two phases, and polycarbonate-based resins have a higher affinity for fillers than polyolefin-based resins, and thus polycarbonate-based resins having a specific phase. It can be significantly present on the resin.
  • the polycarbonate-based resin is excellent in mechanical strength, high heat resistance, transparent, and excellent moldability has the advantage of having excellent physical properties for producing a molded article.
  • Polyolefin resins also have advantages of excellent heat resistance and transparency and light weight.
  • the polymer composition of the present invention contain 10 to 80% by volume of polycarbonate resin.
  • the polycarbonate-based resin is included in the polymer composition in an amount outside the above range, two different phases may not be sufficiently formed, thereby making it difficult to control a desired morphology.
  • the polymer composition of the present invention contains 20 to 70% by volume of polycarbonate resin. Because, when the content of the polycarbonate-based resin is contained in 20 to 70% by volume, not only high thermal conductivity but also excellent processability, thermal conductivity, mechanical properties, thermal stability, etc. can be obtained at a certain level or more suitable for the actual use environment. Because there is.
  • the polycarbonate resin included in the polymer composition of the present invention is preferably a polycarbonate resin based on bisphenol-A, but is not limited thereto.
  • the polymer composition of the present invention contain 10 to 80% by volume of polyolefin resin.
  • the polyolefin-based resin is included in the polymer composition in an amount outside the above range, two different phases are not sufficiently formed, which makes it difficult to control a desired morphology.
  • the polymer composition of the present invention contains 20 to 70% by volume of polyolefin resin. Because, when the content of the polyolefin resin is contained in 20 to 70% by volume, not only high thermal conductivity but also excellent properties such as excellent processability, thermal conductivity, mechanical properties, and thermal stability can be secured to a certain level or more suitable for actual use environments. Because.
  • Polyolefin resins included in the polymer composition of the present invention are ethylene octene rubber (EOR), ethylene propylene rubber (EPR), ethylene-propylene-diene rubber (EPDM), linear low density polyethylene (LLDPE), low density polyethylene (LDPE), high density It is preferably one kind selected from the group consisting of polyethylene (HDPE) and polypropylene (PP), but is not limited thereto.
  • EOR ethylene octene rubber
  • EPR ethylene propylene rubber
  • EPDM ethylene-propylene-diene rubber
  • LLDPE linear low density polyethylene
  • LDPE low density polyethylene
  • HDPE polyethylene
  • PP polypropylene
  • the polymer composition according to the present invention contains 5 to 80% by volume of thermally and electrically conductive fillers.
  • the filler is included in less than 5% by volume, there is a problem that the thermal and electrical conductivity of the composition is significantly lowered, and when it is included in excess of 80% by volume, the viscosity of the composition is too high and the moldability is significantly lowered, There is also a problem that the mechanical strength of the molded article is also significantly reduced.
  • the polymer composition of the present invention contains 10 to 60% by volume of thermal and electrically conductive fillers.
  • the thermally conductive filler included in the polymer composition according to the present invention is preferably a carbon-based filler, and more preferably graphite, but is not limited thereto as long as the filler has high thermal conductivity.
  • Graphite is suitable for use as a filler in the polymer composition of the present invention because it exhibits a very high thermal conductivity of 400 W / (m ⁇ K) or more.
  • the present invention is 10 to 80% by volume of a polycarbonate resin; 10 to 80% by volume polyolefin resin; And 5 to 80% by volume of thermal and electrically conductive fillers.
  • the polymer composition constituting the composition as described above using conventional molding apparatuses such as a conventional extruder, Brabender Plasticorder, Banbury Mixer, Kneader or Roll Mill It can be produced by melt mixing at 250 to 350 °C 10 to 500 rpm.
  • the polymer composition according to the present invention includes a polymer having excellent moldability and includes a filler in a range that does not impair moldability, there is an advantage in that workability is very excellent in molding it by a method such as injection molding.
  • the molded article produced by this has the advantage of excellent thermal conductivity as well as mechanical strength.
  • the molded article according to the present invention may be applied to a component for releasing heat generated from an electronic device due to excellent thermal conductivity, but is not necessarily limited thereto.
  • step 2 Mixing 10 to 80% by volume polycarbonate resin, 10 to 80% by volume polyolefin resin, and 5 to 80% by volume thermally conductive filler (step 1); And hot-extruding the mixed mixture (step 2).
  • step by step the manufacturing method of the present invention will be described in detail step by step the manufacturing method of the present invention.
  • Step 1 of the preparation method of the present invention is a step of mixing 10 to 80% by volume of the polycarbonate resin, 10 to 80% by volume of the polyolefin resin, and 5 to 80% by volume of the thermally conductive filler.
  • the polycarbonate-based resin, the polyolefin-based resin and the thermally conductive filler in the form of particles are uniformly mixed at room temperature.
  • Step 2 of the manufacturing method of the present invention is a step of hot extrusion of the uniformly mixed mixture.
  • Hot extrusion of the mixture can be carried out according to known methods using a device such as, for example, a twin-screw extruder.
  • the polycarbonate resin and the polyolefin resin are not compatible with each other, and thus, two different phases are formed during the mixing process. Among these, the polycarbonate resin has a high affinity for the filler, and thus the filler is formed by the polycarbonate resin. There is a significant amount present in the phase.
  • the mixing of the resin and the filler is an environmentally friendly process because it proceeds by the normal temperature mixing and melting process of the particles, since no solvent is used at all, the modification of the filler is not necessary, and the mixing is possible by a simple method. Can be simplified, and productivity is improved.
  • the polycarbonate resin used in the production method of the present invention is preferably a polycarbonate resin based on bisphenol-A, but is not limited thereto.
  • the polyolefin resin used in the same step is ethylene octene rubber (EOR), ethylene propylene rubber (EPR), ethylene-propylene-diene rubber (EPDM), linear low density polyethylene (LLDPE), low density polyethylene (LDPE), high density polyethylene (HDPE), and polypropylene (PP) is preferably one selected from the group consisting of, but is not limited thereto.
  • the thermally conductive filler used in the same step is preferably a carbon-based filler, more preferably graphite, but is not limited thereto as long as the filler has high thermal conductivity.
  • Graphite is suitable for use as a filler in the polymer composition of the present invention because it exhibits a very high thermal conductivity of 400 W / (m ⁇ K) or more.
  • the content of the polycarbonate resin, polyolefin resin, and thermal and electrical conductivity fillers mixed in the manufacturing step of the present invention is 20 to 70% by volume, 20 to 70% by volume, and 10 to 60% by volume, respectively. desirable. This is because not only high thermal conductivity but also excellent processability, thermal conductivity, mechanical properties, and thermal stability in the resin content can be secured to a certain level or more suitable for actual use environments.
  • Extrusion process of the present invention is preferably carried out at a temperature of 250 to 350 °C. If the temperature at the time of extrusion is less than 250 °C there is a problem that the mixing between the resin and the filler is not sufficiently made, if the temperature exceeds 350 °C there is a problem that the physical properties are degraded due to the thermal decomposition of the resin.
  • step A Mixing 10 to 80% by volume polycarbonate resin, 10 to 80% by volume polyolefin resin, and 5 to 80% by volume thermally conductive filler (step A);
  • It provides a method for producing a molded article comprising a polymer composition comprising the step (step C) injection molding the extrudate.
  • the desired molded article may be manufactured by injection molding the polymer composition prepared according to the method of preparing the polymer composition as described in Step C.
  • Steps A and B for preparing the polymer composition are the same as steps 1 and 2 of the method for preparing the polymer, and description thereof is omitted.
  • the injection molding of step C of the manufacturing method of the present invention can be performed by a known method using a device such as an injection molding machine.
  • the molded article including the polymer composition prepared by the manufacturing method of the present invention is used for the purpose of releasing heat of the electronic device due to its excellent mechanical strength and excellent thermal conductivity, and can be usefully applied to a component that should have electrical conductivity.
  • a pellet of the polymer composition was prepared in the same manner as in Example 1, except that 20% by volume of the polycarbonate resin, 30% by volume of the polyolefin resin, and 50% by volume of the filler were mixed.
  • a pellet of a polymer composition was prepared in the same manner as in Example 1, except that 24 vol% of a polycarbonate resin, 36 vol% of a polyolefin resin, and 40 vol% of a filler were mixed.
  • a pellet of the polymer composition was prepared in the same manner as in Comparative Example 1, except that 65 vol% of the polycarbonate resin and 35 vol% of the filler were mixed.
  • a pellet of the polymer composition was prepared in the same manner as in Comparative Example 1, except that 73 vol% of the polycarbonate resin and 27 vol% of the filler were mixed.
  • a pellet of the polymer composition was manufactured in the same manner as in Comparative Example 4, except that 50 vol% of the polyolefin resin and 50 vol% of the filler were mixed.
  • a pellet of the polymer composition was prepared in the same manner as in Comparative Example 4, except that 60 vol% of the polyolefin resin and 40 vol% of the filler were mixed.
  • Example 1-Example 3 Each component composition of the said Example 1-Example 3, and Comparative Examples 1-6 was put together in following Table 1.
  • Thermal conductivity ( ⁇ ) thermal diffusivity ( ⁇ ) ⁇ specific heat (Cp) ⁇ density ( ⁇ )
  • the thermal diffusivity of the polymer composition pellets prepared according to Examples 1 to 3 and Comparative Examples 1 to 3 of the present invention was measured according to ASTM E1461 at a temperature of 25 ° C. using a Netzsch LFA 477 measuring instrument (Netzsch).
  • the specific heat was measured according to ASTM E1952 using an MDSC measuring instrument (TA instrument), and the density was measured according to ASTM D6226 using a Gas Pycnometer (Protech).
  • Thermal conductivity was calculated from the measured thermal diffusivity, specific heat, and density of each polymer composition pellet using Equation 1, and the results are shown in Table 2 below.
  • the polymer composition according to the present invention has excellent thermal conductivity.
  • the thermal conductivity of the polymer composition of Example 2 is 30 times higher.
  • the impact strength of the polymer composition pellets prepared according to Examples 1 to 3 and Comparative Examples 1 to 3 of the present invention was measured according to ASTM D256 using an Izod impact strength tester (Izod type impact strength tester). The results are shown in Table 3 below.
  • the polymer composition according to the present invention can be seen that the impact strength is very low while having a very good thermal conductivity.
  • the thermal conductivity of the polymer composition of Example 1 is four times higher, it can be seen that the impact strength is similar.
  • Comparative Example 4-6 injection molding was not possible, and thus the impact strength was not measured.

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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)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Processes Of Treating Macromolecular Substances (AREA)

Abstract

L'invention concerne une composition de polymère dotée d'une bonne conductivité thermique supérieure, un moule fabriqué à partir de ladite composition de polymère et un procédé de fabrication de la composition et du moule précités. En particulier, l'invention se rapporte à une composition de polymère qui renferme de 10 à 80% volumique d'une résine à base de polycarbonate, de 10 à 80% volumique d'une résine à base de polyoléfine et de 5 à 80% volumique d'une charge thermo-conductrice, ainsi qu'à un moule fabriqué à partir de ladite composition. L'invention porte aussi sur un procédé de préparation de ladite composition de polymère, lequel procédé consiste à mélanger de 10 à 80% volumique d'une résine à base de polycarbonate, de 10 à 80% volumique d'une résine à base de polyoléfine et de 5 à 80% volumique d'une charge thermo-conductrice, et à extruder le mélange obtenu. L'invention permet, en régulant la morphologie des polymères dans la composition, cela même lorsqu'une seule sorte de charge est utilisée, de former un réseau efficace entre les charges, ce qui augmente considérablement la conductivité thermique de la composition de polymère. Le moule fabriqué à partir de la composition de polymère selon l'invention trouve une application utile comme composant dans divers produits tels que les puits thermiques pour instruments électroniques.
PCT/KR2012/001662 2011-05-19 2012-03-07 Composition de polymère possédant une bonne conductivité thermique supérieure et procédé de préparation de ladite composition Ceased WO2012157841A1 (fr)

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KR10-2011-0047283 2011-05-19
KR1020110047283A KR101285349B1 (ko) 2011-05-19 2011-05-19 열전도성이 우수한 고분자 조성물 및 이의 제조방법

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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0428042A2 (fr) * 1989-11-13 1991-05-22 Mitsubishi Chemical Corporation Composition de résine thermoplastique conductible
JPH07157601A (ja) * 1993-10-15 1995-06-20 Sumitomo Bakelite Co Ltd 導電性非晶性ポリオレフィン樹脂組成物
US20080234434A1 (en) * 2007-03-20 2008-09-25 Ye-Gang Lin Polycarbonate/polyolefin based resin compositions and their production processes and uses
KR20100058342A (ko) * 2008-11-24 2010-06-03 한화케미칼 주식회사 복합탄소소재를 포함하는 전도성 수지조성물

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0428042A2 (fr) * 1989-11-13 1991-05-22 Mitsubishi Chemical Corporation Composition de résine thermoplastique conductible
JPH07157601A (ja) * 1993-10-15 1995-06-20 Sumitomo Bakelite Co Ltd 導電性非晶性ポリオレフィン樹脂組成物
US20080234434A1 (en) * 2007-03-20 2008-09-25 Ye-Gang Lin Polycarbonate/polyolefin based resin compositions and their production processes and uses
KR20100058342A (ko) * 2008-11-24 2010-06-03 한화케미칼 주식회사 복합탄소소재를 포함하는 전도성 수지조성물

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KR101285349B1 (ko) 2013-07-10

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