KR102180206B1 - Thermal conductive polymer composites comprising aluminum and carbon material and their application of heat dissipation products - Google Patents

Thermal conductive polymer composites comprising aluminum and carbon material and their application of heat dissipation products Download PDF

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KR102180206B1
KR102180206B1 KR1020190063157A KR20190063157A KR102180206B1 KR 102180206 B1 KR102180206 B1 KR 102180206B1 KR 1020190063157 A KR1020190063157 A KR 1020190063157A KR 20190063157 A KR20190063157 A KR 20190063157A KR 102180206 B1 KR102180206 B1 KR 102180206B1
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thermally conductive
aluminum
polymer composite
composite composition
carbon material
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오원태
송치호
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동의대학교 산학협력단
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    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00Use of inorganic substances as compounding ingredients
    • C08K3/02Elements
    • C08K3/08Metals
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    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08JWORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J5/00Manufacture of articles or shaped materials containing macromolecular substances
    • C08J5/18Manufacture of films or sheets
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00Use of inorganic substances as compounding ingredients
    • C08K3/02Elements
    • C08K3/04Carbon
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K7/00Use of ingredients characterised by shape
    • C08K7/02Fibres or whiskers
    • C08K7/04Fibres or whiskers inorganic
    • C08K7/06Elements
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L33/00Compositions of homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and only one being terminated by only one carboxyl radical, or of salts, anhydrides, esters, amides, imides or nitriles thereof; Compositions of derivatives of such polymers
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    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J9/00Adhesives characterised by their physical nature or the effects produced, e.g. glue sticks
    • DTEXTILES; PAPER
    • D01NATURAL OR MAN-MADE THREADS OR FIBRES; SPINNING
    • D01FCHEMICAL FEATURES IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS; APPARATUS SPECIALLY ADAPTED FOR THE MANUFACTURE OF CARBON FILAMENTS
    • D01F9/00Artificial filaments or the like of other substances; Manufacture thereof; Apparatus specially adapted for the manufacture of carbon filaments
    • D01F9/08Artificial filaments or the like of other substances; Manufacture thereof; Apparatus specially adapted for the manufacture of carbon filaments of inorganic material
    • D01F9/12Carbon filaments; Apparatus specially adapted for the manufacture thereof
    • D01F9/14Carbon filaments; Apparatus specially adapted for the manufacture thereof by decomposition of organic filaments
    • D01F9/145Carbon filaments; Apparatus specially adapted for the manufacture thereof by decomposition of organic filaments from pitch or distillation residues
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00Use of inorganic substances as compounding ingredients
    • C08K3/02Elements
    • C08K3/08Metals
    • C08K2003/0812Aluminium
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    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K2201/00Specific properties of additives
    • C08K2201/001Conductive additives
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    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K2201/00Specific properties of additives
    • C08K2201/002Physical properties
    • C08K2201/003Additives being defined by their diameter
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K2201/00Specific properties of additives
    • C08K2201/002Physical properties
    • C08K2201/005Additives being defined by their particle size in general
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J2301/00Additional features of adhesives in the form of films or foils
    • C09J2301/30Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier
    • C09J2301/314Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier the adhesive layer and/or the carrier being conductive

Abstract

The present invention relates to a polymer composite composition comprising aluminum and a carbon material. More particularly, the present invention relates to a thermally conductive polymer composite composition including an acrylic resin, aluminum, and a carbon material, and a thermally conductive adhesive, film, and tape including the same. The thermally conductive polymer composite composition according to the present invention has an effect of improving heat dissipation properties (vertical thermal conductivity) by mixing and using the acrylic resin, aluminum, and carbon material at a specific mixing ratio and, in particular, has an effect of exhibiting excellent heat conduction characteristics while having remarkably low electrical conductivity by using only a small amount of the carbon material.

Description

알루미늄 및 탄소소재를 포함하는 열전도성 고분자 복합 조성물 및 이를 이용한 방열 제품{Thermal conductive polymer composites comprising aluminum and carbon material and their application of heat dissipation products}Thermal conductive polymer composites comprising aluminum and carbon material and their application of heat dissipation products

본 발명은 알루미늄 및 탄소소재를 포함하는 고분자 복합 조성물 및 이를 이용한 방열 제품에 관한 것으로, 구체적으로는 아크릴 수지, 알루미늄 및 탄소소재를 포함하는 열전도성 고분자 복합 조성물 및 이를 포함하는 열전도성 접착제, 필름 및 테이프에 관한 것이다.The present invention relates to a polymer composite composition comprising aluminum and a carbon material, and a heat dissipation product using the same, and specifically, a thermally conductive polymer composite composition comprising an acrylic resin, aluminum and carbon material, and a thermally conductive adhesive, film and It's about tape.

최근 전자 소자의 고집적화로 인해 열 밀도가 급격히 증가하여 전자부품의 수명과 신뢰성에 큰 영향을 미치고 있다. 기존에 개발 된 복합조성물을 사용한 열전도성 충진제 Thermal interface material(TIM)의 경우 반영구적이지 않고 제품의 변형이 생겨 전자제품에 사용되기에는 어려움이 있다. 따라서 최근 열전도 점착 시트, 필름, 열전도성 테이프 등 제품이 개발되고 있다.Recently, due to the high integration of electronic devices, the thermal density increases rapidly, which has a great influence on the life and reliability of electronic components. Thermal interface material (TIM), a thermally conductive filler using a previously developed composite composition, is not semi-permanent and is difficult to use in electronic products due to product deformation. Accordingly, products such as thermally conductive adhesive sheets, films, and thermally conductive tapes have recently been developed.

제품에 사용되는 방열 소재로는 세라믹, 탄소, 금속 소재 등 열전도성 필러와 고분자로 이루어진 복합재료를 사용하는 경우가 늘어나고 있다. 기존 시장에 무기재료를 사용한 복합조성물의 경우 1~2W/mK 사이의 열전도도를 가지고 있고 금속 소재를 사용한 경우는 3W/mK 내외의 열전도 특성을 보유하고 있다. 향후 전기 및 전자기기의 고성능화로 인해 발열문제가 더 심각해지는 문제를 해결하기 위해 더 높은 열전도 특성과 안정적인 점착특성을 갖춘 기능소재의 개발이 요구된다.As heat dissipation materials used in products, composite materials made of thermally conductive fillers and polymers such as ceramic, carbon, and metal materials are increasingly used. Composite compositions using inorganic materials in the existing market have thermal conductivity between 1 and 2W/mK, and when using metal materials, they have thermal conductivity properties of around 3W/mK. In order to solve the problem that the heating problem becomes more serious due to the high performance of electric and electronic devices in the future, the development of functional materials with higher heat conduction characteristics and stable adhesion characteristics is required.

기존에 사용되는 무기재료를 이용한 복합조성물의 경우, 소재 자체의 열전도성이 크지 않기 때문에, 고열전도 특성을 확보하기 힘들다. 탄소소재의 경우 소재 자체의 열전도 특성은 우수하나 구조적으로 수직 방향 열전도도가 우수하지 않으며, 첨가량이 너무 많을 경우 점착력에 문제가 생긴다. 무기재료에 탄소소재의 첨가하여 구조적 변화와 수직 방향 열전도 특성을 향상시켜도 열전도 특성이 크게 증가하지는 않으며, 향후 더 고성능의 전자제품에 사용하기에는 열전도 특성이 미흡한 수준이다. 은(Ag) 또는 구리(Cu)과 같은 고열전도성 소재를 첨가하여 고열전도 특성을 확보하려는 시도도 있었으나, 상기 소재는 고가의 제품으로, 시장에 상용화되기에는 어려움이 있다. 또한, 높은 열전도성이지만 전기전도특성 때문에 전자기기에 적용하기에는 기술적으로 여러 문제점이 나타난다. 따라서, 좋은 방열필러를 사용하는 것 뿐만 아니라 소재 자체가 가지고 있는 열전도 특성도 중요하며 소재 각각의 장점을 이용하여 열전도 특성을 크게 향상 시킬 수 있는 기술이 필요하다.In the case of a composite composition using an inorganic material that has been used, it is difficult to secure high thermal conductivity characteristics because the thermal conductivity of the material itself is not large. In the case of carbon materials, the thermal conductivity of the material itself is excellent, but structurally, the thermal conductivity in the vertical direction is not excellent, and if the amount of addition is too large, a problem occurs in adhesion. Even if the structural change and vertical heat conduction characteristics are improved by adding carbon materials to inorganic materials, the heat conduction characteristics do not increase significantly, and the heat conduction characteristics are insufficient for use in higher-performance electronic products in the future. There have been attempts to secure high thermal conductivity by adding a high thermal conductivity material such as silver (Ag) or copper (Cu), but the material is an expensive product, and it is difficult to commercialize it in the market. In addition, although it has high thermal conductivity, there are technical problems when it is applied to electronic devices due to its electrical conductivity. Therefore, not only the use of good heat dissipation fillers, but also the heat conduction characteristics of the material itself are important, and a technology that can greatly improve the heat conduction characteristics by using the advantages of each material is required.

이에, 본 발명자들은 고열전도성 소재인 금속파우더와 탄소소재를 첨가한 고분자 복합 조성물에 대하여 연구한 결과, 아크릴 수지, 알루미늄 및 탄소소재를 특정 혼합비율로 혼합하여 사용함에 따라서 절연특성을 가지면서도 방열 특성(수직 열전도성)이 향상되는 효과가 있음을 알아내고 본 발명을 완성하였다.Accordingly, the present inventors studied a polymer composite composition in which a metal powder and a carbon material, which is a high thermal conductivity material, are added, and as a result of using an acrylic resin, aluminum, and carbon material by mixing at a specific mixing ratio, it has insulating properties and heat dissipation properties It was found that there is an effect of improving (vertical thermal conductivity) and the present invention was completed.

대한민국 공개특허 10-2015-0140125Republic of Korea Patent Publication 10-2015-0140125

본 발명의 목적은 열전도성 고분자 복합 조성물을 제공하는 것이다.An object of the present invention is to provide a thermally conductive polymer composite composition.

본 발명의 다른 목적은 상기 열전도성 고분자 복합 조성물을 포함하는 열전도성 접착제, 필름 및 테이프를 제공하는 것이다.Another object of the present invention is to provide a thermally conductive adhesive, film and tape comprising the thermally conductive polymer composite composition.

상기 목적을 달성하기 위하여,To achieve the above object,

본 발명은 고분자 수지 40 중량부 기준;The present invention based on 40 parts by weight of a polymer resin;

열전도성 금속 필러 58 내지 59.5 중량부; 및58 to 59.5 parts by weight of a thermally conductive metal filler; And

열전도성 탄소 필러 0.5 내지 2 중량부;를 포함하는,Including 0.5 to 2 parts by weight of a thermally conductive carbon filler,

열전도성 고분자 복합 조성물을 제공한다.It provides a thermally conductive polymer composite composition.

본 발명의 일실시예에 있어서, 상기 고분자 수지는 아크릴 수지일 수 잇고, 상기 열전도성 금속 필러는 알루미늄(Al2O3)일 수 있고, 상기 열전도성 탄소 필러는 천연 흑연, 등방성 흑연 및 탄소 섬유로 이루어진 군으로부터 선택된 1종 이상인 것일 수 있다.In one embodiment of the present invention, the polymer resin may be an acrylic resin, the thermally conductive metal filler may be aluminum (Al 2 O 3 ), and the thermally conductive carbon filler may be natural graphite, isotropic graphite, and carbon fiber. It may be one or more selected from the group consisting of.

또한, 본 발명은 상기 열전도성 고분자 복합 조성물을 포함하는 열전도성 접착제, 필름 및 테이프를 제공한다.In addition, the present invention provides a thermally conductive adhesive, film, and tape comprising the thermally conductive polymer composite composition.

본 발명에 따른 열전도성 고분자 복합 조성물은 아크릴 수지, 알루미늄 및 탄소소재를 특정 혼합비율로 혼합하여 사용함에 따라서, 방열 특성(수직 열전도성)이 향상되는 효과가 있고, 특히, 탄소소재를 소량만 사용함에 따라서 전기전도도가 현저히 낮으면서도 우수한 열전도 특성을 나타낼 수 있는 효과가 있다.The thermally conductive polymer composite composition according to the present invention has an effect of improving heat dissipation properties (vertical thermal conductivity) by mixing acrylic resin, aluminum and carbon materials at a specific mixing ratio, and in particular, only a small amount of carbon materials is used. Accordingly, there is an effect of exhibiting excellent heat conduction characteristics while having remarkably low electrical conductivity.

도 1은 아크릴 수지 바인더 단독 소재(a) 및 구상 입자를 가진 알루미늄 및 탄소섬유가 포함된 조성물(b)의 입자 배열 구조를 나타낸 모식도이다.
도 2는 알루미늄(a), 구리(b), 니켈(c) 금속소재와 본 발명에 따른 실시예 3-3의 고분자 복합 조성물(d)의 구조를 확인한 SEM 촬영 이미지이다.
1 is a schematic diagram showing a particle arrangement structure of an acrylic resin binder alone material (a) and a composition (b) containing aluminum and carbon fibers having spherical particles.
FIG. 2 is a SEM image showing the structures of aluminum (a), copper (b), nickel (c) metal materials and the polymer composite composition (d) of Example 3-3 according to the present invention.

본 발명에서 사용되는 모든 기술용어는, 달리 정의되지 않는 이상, 하기의 정의를 가지며 본 발명의 관련 분야에서 통상의 당업자가 일반적으로 이해하는 바와 같은 의미에 부합된다 또한, 본 명세서에는 바람직한 방법이나 시료가 기재되나, 이와 유사하거나 동등한 것들도 본 발명의 범주에 포함된다 본 명세서에 참고문헌으로 기재되는 모든 간행물의 내용은 본 발명에 도입된다.All technical terms used in the present invention, unless otherwise defined, have the following definitions and correspond to the meaning as commonly understood by those of ordinary skill in the relevant fields of the present invention. In addition, in the present specification, preferred methods or samples Is described, but similar or equivalents thereof are also included in the scope of the present invention. The contents of all publications referred to herein by reference are incorporated into the present invention.

용어 "약"이라는 것은 참조 양, 수준, 값, 수, 빈도, 퍼센트, 치수, 크기, 양, 중량 또는 길이에 대해 30, 25, 20, 25, 10, 9, 8, 7, 6, 5, 4, 3, 2 또는 1% 정도로 변하는 양, 수준, 값, 수, 빈도, 퍼센트, 치수, 크기,양, 중량 또는 길이를 의미한다.The term “about” refers to 30, 25, 20, 25, 10, 9, 8, 7, 6, 5, or 30, 25, 20, 25, 10, 9, 8, 7, 6, 5, or relative to a reference amount, level, value, number, frequency, percentage, dimension, size, amount, weight or length. It means an amount, level, value, number, frequency, percentage, dimension, size, amount, weight or length varying by 4, 3, 2 or 1%.

본 명세서를 통해, 문맥에서 달리 필요하지 않으면, "포함하다" 및 "포함하는"이란 말은 제시된 단계 또는 구성요소, 또는 단계 또는 구성요소들의 군을 포함하나, 임의의 다른 단계 또는 구성요소, 또는 단계 또는 구성요소들의 군이 배제되지는 않음을 내포하는 것으로 이해하여야 한다.Throughout this specification, unless otherwise required by the context, the terms “comprise” and “comprising” include the steps or components presented, or groups of steps or components, but any other step or component, or It is to be understood that a step or group of components is not excluded.

일반적으로, 알루미늄과 탄소소재를 포함하는 고분자 복합소재를 연구 개발 할 때 절연, 열전도 특성, 생산비용 등 고려하는 스펙에 따라 조성비 선택의 기준이 된다. 구체적으로 탄소소재 자체의 열전도도는 흑연(Graphite)과 탄소섬유(Carbon fiber; CF)의 경우 각각 ~200W/mK, ~800W/mK 수준으로 무기필러인 알루미늄보다 탄소소재가 월등히 높다. 하지만 자체의 열전도 특성이 좋은 탄소소재를 많이 첨가한다고 열전도도가 더 우수하지 않으며, 알루미늄 또는 탄소소재를 각각 단독으로 함량을 많이 첨가하여도 우수한 열전도 특성이 나타나지 않는다. 알루미늄 단독으로 사용할 경우 입자사이의 빈공간이 생기게 돼서 열전도 특성이 떨어지고 탄소필러를 단독으로 사용할 경우 침상구조나 판상구조로 입자사이 빈 공간은 적으나 수직방향으로 열을 전달 할 때 너무 많은 입자를 거치기 때문에 수직 방향으로 열전도 효율이 좋을 수 없다(도 1 참조).In general, when researching and developing a polymer composite material containing aluminum and carbon materials, it is a criterion for selecting a composition ratio according to specifications that take into account insulation, heat conduction properties, and production costs. Specifically, the thermal conductivity of the carbon material itself is ~200W/mK and ~800W/mK in the case of graphite and carbon fiber (CF), respectively, and the carbon material is far higher than that of aluminum, which is an inorganic filler. However, the addition of a large number of carbon materials with good thermal conductivity properties does not provide better thermal conductivity, and even if a large amount of aluminum or carbon materials are added alone, excellent thermal conductivity properties do not appear. When aluminum is used alone, heat conduction characteristics are degraded due to the creation of voids between particles. When carbon fillers are used alone, there are few voids between particles due to a needle-like structure or a plate-like structure, but too many particles pass through when heat is transferred in a vertical direction. Therefore, the heat conduction efficiency in the vertical direction cannot be good (see Fig. 1).

이에, 본 발명자들은 알루미늄과 탄소소재를 첨가한 고분자 복합 조성물을 제조할 때 가장 열전도 특성이 좋은 조성비를 연구한 결과, 탄소 소재를 소량만 첨가하여도, 특정 조성비에서 알루미늄 입자사이 빈 공간을 유연한 선형 구조를 갖는 탄소소재가 적절하게 잘 이어줌으로써 입자 배열이 잘 형성되어 수직방향 열전도도가 상승할 수 있음을 확인하여 본 발명을 완성하였다.Accordingly, the present inventors studied the composition ratio having the best thermal conductivity when preparing a polymer composite composition containing aluminum and carbon materials. As a result, even if only a small amount of carbon material is added, the empty space between the aluminum particles is flexible and linear. The present invention was completed by confirming that the structured carbon material can be properly connected so that the particle arrangement is well formed and the thermal conductivity in the vertical direction can be increased.

이하, 본 발명을 상세히 설명한다.Hereinafter, the present invention will be described in detail.

열전도성 고분자 복합 조성물Thermally conductive polymer composite composition

본 발명은 고분자 수지 40 중량부 기준;The present invention based on 40 parts by weight of a polymer resin;

열전도성 금속 필러 58 내지 59.5 중량부; 및58 to 59.5 parts by weight of a thermally conductive metal filler; And

열전도성 탄소 필러 0.5 내지 2 중량부;를 포함하는,Including 0.5 to 2 parts by weight of a thermally conductive carbon filler,

열전도성 고분자 복합 조성물을 제공한다.It provides a thermally conductive polymer composite composition.

본 발명에 따른 열전도성 고분자 복합 조성물에 있어서, 상기 고분자 수지는 아크릴 수지인 것일 수 있다. 상기 고분자 수지는 바인더로서 첨가되는 것일 수 있다.In the thermally conductive polymer composite composition according to the present invention, the polymer resin may be an acrylic resin. The polymer resin may be added as a binder.

상기 아크릴 수지로는 올레핀 수지, 폴리 우레탄 수지, 시아노 아크릴레이트 수지, 이소시아네이트 수지, 아크릴공중합체, 메틸메타크릴레이트 등을 사용할 수 있고, 바람직하게는 올레핀 수지 및 아크릴 공중합체로 이루어진 군으로부터 선택되는 1종 이상을 사용하는 것일 수 있다. 본 발명의 일실시예에 따르면, Butyl acrylate(BAM), 2-ethylhexyl acrylate(2-EHAM), Methyl methacrylate(MMA)를 주모노머로 하는 아크릴 공중합체로서, 특히 2-EHAM을 주모노머로 하여 낮은 Tg의 BAM을 사용하고 Tg가 높은 MMA로 stiffness를 증가시킨 아크릴 공중합체를 사용하는 것일 수 있으나, 이에 제한되지는 않는다. 본 발명에 따른 상기 열전도성 고분자 복합 조성물은 다양한 아크릴계 관능 모노머를 접목하기 쉬워 다양한 분야에 사용가능할 수 있다.As the acrylic resin, an olefin resin, a polyurethane resin, a cyano acrylate resin, an isocyanate resin, an acrylic copolymer, a methyl methacrylate, etc. may be used, preferably selected from the group consisting of an olefin resin and an acrylic copolymer. It may be to use more than one type. According to an embodiment of the present invention, as an acrylic copolymer using butyl acrylate (BAM), 2-ethylhexyl acrylate (2-EHAM), and methyl methacrylate (MMA) as the main monomer, in particular, 2-EHAM as the main monomer It may be to use an acrylic copolymer in which stiffness is increased by using Tg of BAM and high Tg of MMA, but is not limited thereto. The thermally conductive polymer composite composition according to the present invention may be easily grafted with various acrylic functional monomers and can be used in various fields.

본 발명에 따른 상기 열전도성 고분자 복합 조성물은 경화제를 더 포함할 수 있다. 상기 경화제는 조성물의 신속한 경화를 돕는 역할을 하는 것으로서, 특별히 한정되지 않는다. 바람직하게는, 이소시아네이트(isocyanate)계 경화제 및 에폭시(epoxy)계 경화제로 이루어지는 군으로부터 선택되는 1종 이상의 경화제를 사용할 수 있다.The thermally conductive polymer composite composition according to the present invention may further include a curing agent. The curing agent is not particularly limited as it serves to help the rapid curing of the composition. Preferably, at least one type of curing agent selected from the group consisting of an isocyanate curing agent and an epoxy curing agent may be used.

본 발명에 따른 열전도성 고분자 복합 조성물에 있어서, 상기 열전도성 금속 필러는 알루미늄(Al)인 것일 수 있다.In the thermally conductive polymer composite composition according to the present invention, the thermally conductive metal filler may be aluminum (Al).

상기 알루미늄는, 평균 입경이 5-20㎛인 것을 사용할 수 있고, 바람직하게는 7-17㎛인 것을 사용할 수 있으며, 1종 이상의 평균 입경을 갖는 알루미늄를 혼합하여 사용할 수도 있다.As the aluminum, those having an average particle diameter of 5-20 μm may be used, preferably those having an average particle diameter of 7-17 μm may be used, and aluminum having an average particle diameter of one or more may be mixed and used.

상기 범위보다 입자사이즈가 작을 경우, 방열 특성(열전도성)이 저하될 수 있고, 입자사이즈가 커질 경우, 침전되거나 분산이 어려운 단점이 있다.If the particle size is smaller than the above range, heat dissipation characteristics (thermal conductivity) may be deteriorated, and when the particle size increases, there is a disadvantage that it is difficult to precipitate or disperse.

본 발명에 따른 열전도성 고분자 복합 조성물에 있어서, 상기 열전도성 탄소 필러는 천연 흑연, 등방성 흑연 및 탄소 섬유로 이루어진 군으로부터 선택된 1종 이상인 것일 수 있고, 상기 탄소 섬유는 피치계(Pitch)계 탄소섬유인 것일 수 있다.In the thermally conductive polymer composite composition according to the present invention, the thermally conductive carbon filler may be one or more selected from the group consisting of natural graphite, isotropic graphite, and carbon fiber, and the carbon fiber is a pitch-based carbon fiber. It can be.

상기 피치계(Pitch)계 탄소섬유는 섬유단면 평균직경이 13-22㎛인 것을 사용할 수 있고, 바람직하게는 14-21㎛인 것을 사용할 수 있다.The pitch-based carbon fiber may have an average diameter of 13-22 µm in cross section, preferably 14-21 µm.

상기 천연흑연은 평균입도 10-14㎛인 것을 사용할 수 있고, 바람직하게는 11-13㎛인 것을 사용할 수 있다.The natural graphite may be used having an average particle size of 10-14㎛, preferably may be used in the 11-13㎛.

상기 등방성 흑연은 평균입도 8-27㎛인 것을 사용할 수 있고, 바람직하게는 9-26㎛인 것을 사용할 수 있다.The isotropic graphite may be used having an average particle size of 8-27㎛, preferably 9-26㎛.

본 발명에 따른 상기 열전도성 고분자 복합 조성물은 바람직하게는, 고분자 수지 40 중량부 기준; 열전도성 금속 필러 58 내지 58.4 중량부; 및 열전도성 탄소 필러 1.6 내지 2 중량부 포함하는 것일 수 있고, 보다 바람직하게는 고분자 수지 40 중량부 기준; 열전도성 금속 필러 58.0 내지 58.2 중량부; 및 열전도성 탄소 필러 1.8 내지 2.0 중량부 포함하는 것일 수 있다.The thermally conductive polymer composite composition according to the present invention is preferably, based on 40 parts by weight of a polymer resin; 58 to 58.4 parts by weight of a thermally conductive metal filler; And 1.6 to 2 parts by weight of a thermally conductive carbon filler, more preferably based on 40 parts by weight of a polymer resin; 58.0 to 58.2 parts by weight of a thermally conductive metal filler; And 1.8 to 2.0 parts by weight of the thermally conductive carbon filler may be included.

또한, 본 발명은 본 발명에 따른 상기 열전도성 고분자 복합 조성물을 포함하는 열전도성 접착체, 열전도성 필름 및 열전도성 테이프를 제공한다.In addition, the present invention provides a thermally conductive adhesive, a thermally conductive film, and a thermally conductive tape including the thermally conductive polymer composite composition according to the present invention.

상기 열전도성 접착제는 시트 형태로도 제조되는 것일 수 있고, 상기 열전도성 필름은 점착 필름일 수 있으나, 이에 제한되지는 않는다.The thermally conductive adhesive may be manufactured in the form of a sheet, and the thermally conductive film may be an adhesive film, but is not limited thereto.

이하, 본 발명을 하기의 실시예에 의하여 더욱 상세하게 설명한다. 단, 하기의 실시예는 본 발명을 예시하는 것일 뿐, 본 발명의 내용이 하기의 실시예에 의해 한정되는 것은 아니다.Hereinafter, the present invention will be described in more detail by the following examples. However, the following examples are merely illustrative of the present invention, and the contents of the present invention are not limited by the following examples.

<실시예 1-1 내지 3-8> 열전도성 고분자 복합 조성물 및 필름의 제조<Examples 1-1 to 3-8> Preparation of thermally conductive polymer composite composition and film

하기 아크릴 수지 및 알루미늄과 다양한 탄소소재를 혼합하여 하기 표 1의 조성으로 열전도성 고분자 복합 조성물을 제조하였다.The following acrylic resin and aluminum were mixed with various carbon materials to prepare a thermally conductive polymer composite composition with the composition shown in Table 1 below.

아크릴 수지: 대흥 특수 화학, Du-1000(아크릴 공중합체);Acrylic resin: Daeheung Special Chemical, Du-1000 (acrylic copolymer);

알루미늄(Al) 분말: Metal player (평균입경 10㎛);Aluminum (Al) powder: Metal player (average particle diameter 10㎛);

흑연 분말(천연흑연): Natural Graphite, S12(평균입도 12㎛);Graphite powder (natural graphite): Natural Graphite, S12 (average particle size 12 µm);

등방성 흑연: 신성카본, 등방성 흑연(평균입도 12㎛); 및Isotropic graphite: new carbon, isotropic graphite (average particle size 12 µm); And

피치계 탄소섬유(CF(pitch)): Mitsubishi Rayon K223HM (섬유단면 직경: 15~20㎛).Pitch-based carbon fiber (CF (pitch)): Mitsubishi Rayon K223HM (fiber cross-section diameter: 15-20㎛).

구체적으로, PE통(200ml)에 저울(HR 200)을 이용하여 바인더(아크릴 수지, 12g)를 넣은 다음 알루미늄(17.10~17.94g), 탄소소재(S12, 등방성 흑연, CF(pitch))를 최소 0.2g 내지 최대 3g을 차례대로 첨가하였다. 구체적인 첨가량은 하기 표 1의 조성과 같다. Paste Mixer를 500rpm(2분 30초), 800rpm(5분 30초), 1000rpm(2분)으로 설정 후 총 10분 간 섞고, 믹싱이 끝난 혼합물은 분산 정도를 확인 후 경화제(바인더의 0.8중량%)를 넣고 혼합하여 실시예 1-1 내지 3-8의 열전도성 고분자 복합조성물을 제조하였다.Specifically, a binder (acrylic resin, 12g) is put in a PE container (200ml) using a balance (HR 200), and then aluminum (17.10-17.94g) and carbon material (S12, isotropic graphite, CF (pitch)) are minimized. 0.2g up to 3g were added in sequence. The specific addition amount is the same as the composition in Table 1 below. After setting the Paste Mixer to 500 rpm (2 minutes 30 seconds), 800 rpm (5 minutes 30 seconds), and 1000 rpm (2 minutes), mix for a total of 10 minutes.After confirming the dispersion degree of the mixture, the curing agent (0.8% by weight of the binder) ) And mixed to prepare a thermally conductive polymer composite composition of Examples 1-1 to 3-8.

실리콘 이형필름에 적정량의 상기 각 복합조성물을 도포한 후 어플리케이터 150㎛로 필름을 제조하였다. 80℃의 드라이 오븐 내에서 5~10분 경화시켜 열전도성 점착 필름을 제조하였다.After applying the appropriate amount of each composite composition to a silicone release film, a film was prepared with an applicator of 150 μm. A thermally conductive adhesive film was prepared by curing for 5 to 10 minutes in a dry oven at 80°C.

하기 표 1은 아크릴 12g을 40 중량부로 하고, 아크릴 첨가량을 기준으로 다른 성분의 첨가량을 중량부로 계산하여 나타내었다.Table 1 shows 12 g of acrylic as 40 parts by weight, and the amount of other components added is calculated in parts by weight based on the amount of acrylic added.

아크릴acryl 알루미늄aluminum 탄소소재Carbon material 아크릴acryl 알루미늄aluminum 탄소소재Carbon material 실시예 1-1Example 1-1 4040 57.057.0 S12S12 3.03.0 실시예 2-5Example 2-5 4040 59.059.0 등방성흑연Isotropic graphite 1.01.0 실시예 1-2Example 1-2 4040 57.557.5 S12S12 2.52.5 실시예 2-6Example 2-6 4040 59.559.5 등방성흑연Isotropic graphite 0.50.5 실시예 1-3Example 1-3 4040 58.058.0 S12S12 2.02.0 실시예 2-7Example 2-7 4040 59.659.6 등방성흑연Isotropic graphite 0.40.4 실시예 1-4Example 1-4 4040 58.258.2 S12S12 1.81.8 실시예 2-8Example 2-8 4040 59.859.8 등방성흑연Isotropic graphite 0.20.2 실시예 1-5Example 1-5 4040 59.059.0 S12S12 1.01.0 실시예 3-1Example 3-1 4040 57.057.0 CF(pitch)CF(pitch) 3.03.0 실시예 1-6Example 1-6 4040 59.559.5 S12S12 0.50.5 실시예 3-2Example 3-2 4040 57.557.5 CF(pitch)CF(pitch) 2.52.5 실시예 1-7Example 1-7 4040 59.659.6 S12S12 0.40.4 실시예 3-3Example 3-3 4040 58.058.0 CF(pitch)CF(pitch) 2.02.0 실시예 1-8Example 1-8 4040 59.859.8 S12S12 0.20.2 실시예 3-4Example 3-4 4040 58.258.2 CF(pitch)CF(pitch) 1.81.8 실시예 2-1Example 2-1 4040 57.057.0 등방성흑연Isotropic graphite 3.03.0 실시예 3-5Example 3-5 4040 59.059.0 CF(pitch)CF(pitch) 1.01.0 실시예 2-2Example 2-2 4040 57.557.5 등방성흑연Isotropic graphite 2.52.5 실시예 3-6Example 3-6 4040 59.559.5 CF(pitch)CF(pitch) 0.50.5 실시예 2-3Example 2-3 4040 58.058.0 등방성흑연Isotropic graphite 2.02.0 실시예 3-7Example 3-7 4040 59.659.6 CF(pitch)CF(pitch) 0.40.4 실시예 2-4Example 2-4 4040 58.258.2 등방성흑연Isotropic graphite 1.81.8 실시예 3-8Example 3-8 4040 59.859.8 CF(pitch)CF(pitch) 0.20.2

<비교예 1-1 내지 3-3> 금속소재를 달리한 열전도성 고분자 복합 조성물 및 필름의 제조<Comparative Examples 1-1 to 3-3> Preparation of a thermally conductive polymer composite composition and film using different metal materials

상기 실시예 1-1 내지 3-8과 동일한 방법으로 고분자 복합 조성물을 제조하되, 알루미늄 대신 하기의 구리, 니켈 또는 알루미나를 이용하여, 하기 표 2의 조성으로 비교예 1-1 내지 3-3의 고분자 복합 조성물을 제조하였다.To prepare a polymer composite composition in the same manner as in Examples 1-1 to 3-8, but using copper, nickel, or alumina instead of aluminum, the composition of Table 2 below was used in Comparative Examples 1-1 to 3-3. A polymer composite composition was prepared.

구리(Cu) 분말: Metal player (평균입경 10㎛);Copper (Cu) powder: Metal player (average particle diameter 10㎛);

니켈(Ni) 분말: Metal player (평균입경 10㎛);Nickel (Ni) powder: Metal player (average particle diameter 10㎛);

알루미나(Al2O3) 분말: Ya'an Bestry Performance materials ALUMINA BAK-20㎛ .Alumina (Al 2 O 3 ) powder: Ya'an Bestry Performance materials ALUMINA BAK-20㎛.

상기 비교예 1-1 내지 3-3의 고분자 복합 조성물을 이용하여 상기 실시예와 동일한 방법으로 열전도성 점착 필름을 제조하였다.Using the polymer composite composition of Comparative Examples 1-1 to 3-3, a thermally conductive adhesive film was prepared in the same manner as in Example.

아크릴acryl 금속소재Metal material 탄소소재Carbon material 비교예 1-1Comparative Example 1-1 4040 CuCu 58.058.0 S12S12 2.02.0 비교예 1-2Comparative Example 1-2 4040 CuCu 58.058.0 등방성흑연Isotropic graphite 2.02.0 비교예 1-3Comparative Example 1-3 4040 CuCu 58.058.0 CF(pitch)CF(pitch) 2.02.0 비교예 2-1Comparative Example 2-1 4040 NiNi 58.058.0 S12S12 2.02.0 비교예 2-2Comparative Example 2-2 4040 NiNi 58.058.0 등방성흑연Isotropic graphite 2.02.0 비교예 2-3Comparative Example 2-3 4040 NiNi 58.058.0 CF(pitch)CF(pitch) 2.02.0 비교예 3-1Comparative Example 3-1 4040 Al2O3 Al 2 O 3 58.058.0 S12S12 2.02.0 비교예 3-2Comparative Example 3-2 4040 Al2O3 Al 2 O 3 58.058.0 등방성흑연Isotropic graphite 2.02.0 비교예 3-3Comparative Example 3-3 4040 Al2O3 Al 2 O 3 58.058.0 CF(pitch)CF(pitch) 2.02.0

<비교예 4 내지 6> 탄소소재 미포함 열전도성 고분자 복합 조성물 및 필름의 제조<Comparative Examples 4 to 6> Preparation of thermally conductive polymer composite composition and film without carbon material

상기 실시예 1-1 내지 3-8 및 비교예 1-1 내지 3-3과 동일한 방법으로 고분자 복합 조성물을 제조하되, 탄소소재를 첨가하지 않고, 아크릴 수지 40 중량부에 금속소재 60 중량부를 하기 표 3과 같이 첨가하여 비교예 4 내지 6의 고분자 복합 조성물을 제조하였다.A polymer composite composition was prepared in the same manner as in Examples 1-1 to 3-8 and Comparative Examples 1-1 to 3-3, but without adding a carbon material, and adding 60 parts by weight of a metal material to 40 parts by weight of an acrylic resin. By adding as shown in Table 3 to prepare a polymer composite composition of Comparative Examples 4 to 6.

상기 비교예 4 내지 6의 고분자 복합 조성물을 이용하여 상기 실시예와 동일한 방법으로 열전도성 점착 필름을 제조하였다.Using the polymer composite composition of Comparative Examples 4 to 6, a thermally conductive adhesive film was prepared in the same manner as in the above Example.

아크릴acryl 금속소재Metal material 탄소소재Carbon material 비교예 4Comparative Example 4 4040 AlAl 6060 00 비교예 5Comparative Example 5 4040 CuCu 6060 00 비교예 6Comparative Example 6 4040 NiNi 6060 00

<실험예 1> 열전도성 고분자 복합 조성물의 열전도도 분석<Experimental Example 1> Analysis of the thermal conductivity of the thermally conductive polymer composite composition

상기 실시예 1-1 내지 3-8 및 비교예 1-1 내지 6의 고분자 복합 조성물의 수직 열전도도(W/m*K)를 ASTM D5470을 이용하여 측정하였고, 하기 표 4에 나타내었다.The vertical thermal conductivity (W/m*K) of the polymer composite compositions of Examples 1-1 to 3-8 and Comparative Examples 1-1 to 6 was measured using ASTM D5470, and is shown in Table 4 below.

구체적으로, 실시예 1-1 내지 3-8 및 비교예 1-1 내지 6의 고분자 복합 조성물을 이용하여 제조된 열전도성 필름에 대하여, 각 샘플의 두께를 측정한 다음, 2.5cm 지름으로 자른 후 3.98mm 두께 구리 지그 사이에 넣고, 0.6kg 하중을 이용해 1차 측정을 실시하였다. 2차 측정은 동일한 샘플을 2장 겹쳐서 1차 측정과 같은 방법을 이용하여 수직 열전도도를 측정하였다. 1차 및 2차 측정시 마다 40번씩 수직 열전도도를 측정하였고, 측정값의 평균값을 최종 결과값으로 하여 하기 표 4에 나타내었다.Specifically, for the thermally conductive films prepared using the polymer composite compositions of Examples 1-1 to 3-8 and Comparative Examples 1-1 to 6, the thickness of each sample was measured, and then cut into a diameter of 2.5 cm. It was put between a 3.98mm thick copper jig, and the primary measurement was performed using a 0.6kg load. For the second measurement, two sheets of the same sample were stacked and the vertical thermal conductivity was measured using the same method as the first measurement. For each of the first and second measurements, the vertical thermal conductivity was measured 40 times, and the average value of the measured values was used as the final result, and is shown in Table 4 below.

금속소재Metal material 탄소소재Carbon material 수직 열전도도
(W/m*K)
Vertical thermal conductivity
(W/m*K)
금속소재Metal material 탄소소재Carbon material 수직 열전도도
(W/m*K)
Vertical thermal conductivity
(W/m*K)
실시예 1-1Example 1-1 AlAl S12S12 3.03.0 2.0492.049 비교예 1-1Comparative Example 1-1 CuCu S12S12 2.02.0 1.7131.713 실시예 1-2Example 1-2 AlAl S12S12 2.52.5 2.5652.565 비교예 1-2Comparative Example 1-2 CuCu 등방성흑연Isotropic graphite 2.02.0 2.2882.288 실시예 1-3Example 1-3 AlAl S12S12 2.02.0 4.0344.034 비교예 1-3Comparative Example 1-3 CuCu CF(pitch)CF(pitch) 2.02.0 1.8311.831 실시예 1-4Example 1-4 AlAl S12S12 1.81.8 3.9823.982 비교예 2-1Comparative Example 2-1 NiNi S12S12 2.02.0 1.3261.326 실시예 1-5Example 1-5 AlAl S12S12 1.01.0 3.5643.564 비교예 2-2Comparative Example 2-2 NiNi 등방성흑연Isotropic graphite 2.02.0 1.7711.771 실시예 1-6Example 1-6 AlAl S12S12 0.50.5 3.5523.552 비교예 2-3Comparative Example 2-3 NiNi CF(pitch)CF(pitch) 2.02.0 1.4181.418 실시예 1-7Example 1-7 AlAl S12S12 0.40.4 2.6622.662 비교예 3-1Comparative Example 3-1 Al2O3 Al 2 O 3 S12S12 2.02.0 1.3351.335 실시예 1-8Example 1-8 AlAl S12S12 0.20.2 2.2782.278 비교예 3-2Comparative Example 3-2 Al2O3 Al 2 O 3 등방성흑연Isotropic graphite 2.02.0 1.5721.572 실시예 2-1Example 2-1 AlAl 등방성흑연Isotropic graphite 3.03.0 2.7942.794 비교예 3-3Comparative Example 3-3 Al2O3 Al 2 O 3 CF(pitch)CF(pitch) 2.02.0 1.9971.997 실시예 2-2Example 2-2 AlAl 등방성흑연Isotropic graphite 2.52.5 2.9852.985 비교예 4Comparative Example 4 AlAl -- -- 3.5473.547 실시예 2-3Example 2-3 AlAl 등방성흑연Isotropic graphite 2.02.0 4.3494.349 비교예 5Comparative Example 5 CuCu -- -- 2.7212.721 실시예 2-4Example 2-4 AlAl 등방성흑연Isotropic graphite 1.81.8 4.2214.221 비교예 6Comparative Example 6 NiNi -- -- 1.6711.671 실시예 2-5Example 2-5 AlAl 등방성흑연Isotropic graphite 1.01.0 3.7283.728 실시예 2-6Example 2-6 AlAl 등방성흑연Isotropic graphite 0.50.5 3.6433.643 실시예 2-7Example 2-7 AlAl 등방성흑연Isotropic graphite 0.40.4 2.9522.952 실시예 2-8Example 2-8 AlAl 등방성흑연Isotropic graphite 0.20.2 2.8262.826 실시예 3-1Example 3-1 AlAl CF(pitch)CF(pitch) 3.03.0 3.5493.549 실시예 3-2Example 3-2 AlAl CF(pitch)CF(pitch) 2.52.5 3.5683.568 실시예 3-3Example 3-3 AlAl CF(pitch)CF(pitch) 2.02.0 5.6495.649 실시예 3-4Example 3-4 AlAl CF(pitch)CF(pitch) 1.81.8 5.5825.582 실시예 3-5Example 3-5 AlAl CF(pitch)CF(pitch) 1.01.0 4.7864.786 실시예 3-6Example 3-6 AlAl CF(pitch)CF(pitch) 0.50.5 4.6724.672 실시예 3-7Example 3-7 AlAl CF(pitch)CF(pitch) 0.40.4 3.6213.621 실시예 3-8Example 3-8 AlAl CF(pitch)CF(pitch) 0.20.2 3.5863.586

상기 표 4에 나타난 바와 같이, 알루미늄을 사용한 경우, 구리, 니켈 또는 알루미나를 사용한 경우보다 더 높은 열전도특성을 나타내었다. 구리, 니켈을 단독을 사용한 경우(비교예 5 및 6) 대비 상기 금속에 탄소소재를 첨가한 경우(비교예 1-1 내지 3-3)에 열전도도가 반감된 반면, 알루미늄를 단독으로 사용했을 때(비교예 4)보다 알루미늄에 다양한 종류의 탄소소재를 첨가하였을 때(실시예 1-1 내지 3-8) 수직방향 열전도도가 대체적으로 향상되었다. 탄소소재를 0.5~2.0중량부 범위 이하 또는 이상의 함량으로 첨가시에는 비교예 4 대비 수직 열전도도의 차이가 크지 않거나 일부 감소되었고, 각 탄소소재를 0.5~2중량부의 함량으로 첨가 했을 때 수직방향 열전도 특성이 더 우수하였으며, 특히, 알루미늄 58.0~58.2 중량부 및 CF(pitch)를 1.8~2중량부 함량으로 첨가한 경우에 5~6W/mk 수준으로 열전도 특성이 크게 상승하였다.As shown in Table 4, when aluminum was used, higher thermal conductivity properties were exhibited than when using copper, nickel, or alumina. When copper and nickel were used alone (Comparative Examples 5 and 6), the thermal conductivity was halved when a carbon material was added to the metal (Comparative Examples 1-1 to 3-3), whereas when aluminum was used alone When various types of carbon materials were added to aluminum than (Comparative Example 4) (Examples 1-1 to 3-8), thermal conductivity in the vertical direction was generally improved. When the carbon material was added in an amount less than or equal to 0.5 to 2.0 parts by weight, the difference in vertical thermal conductivity was not large or partially decreased compared to Comparative Example 4, and when each carbon material was added in an amount of 0.5 to 2 parts by weight, vertical heat conduction The properties were better, and in particular, when 58.0 to 58.2 parts by weight of aluminum and 1.8 to 2 parts by weight of CF (pitch) were added, the heat conduction property was greatly increased to a level of 5 to 6 W/mk.

<실험예 2> 열전도성 고분자 복합 조성물의 구조적 특성 분석<Experimental Example 2> Analysis of the structural properties of the thermally conductive polymer composite composition

상기 실시예 3-3의 고분자 복합 조성물과 알루미늄(Al), 구리(Cu) 및 니켈(Ni) 각 금속소재 파우더를 SEM으로 촬영한 이미지를 도 2에 나타내었다.2 shows an image of the polymer composite composition of Example 3-3 and powders of aluminum (Al), copper (Cu), and nickel (Ni) metal materials, respectively, taken by SEM.

도 2는 알루미늄(a), 구리(b), 니켈(c) 금속소재와 본 발명에 따른 실시예 3-3의 고분자 복합 조성물(d)의 구조를 확인한 SEM 촬영 이미지이다.FIG. 2 is an SEM photographed image confirming the structures of aluminum (a), copper (b), and nickel (c) metal materials and the polymer composite composition (d) of Example 3-3 according to the present invention.

알루미늄 금속파우더(도 2a)는 완전한 구상의 형태로 입자크기는 7~15㎛였고 구리(도 2b)는 뜯어진 모양의 변형 형태로 3~10㎛ 형태를 이루고 있으며 니켈(도 2c)은 3~18㎛ 입자크기로 구상이나 알루미늄만큼의 완전한 구상형태를 가지고 있지 않았다. 실시예 3-3의 고분자 복합 조성물(도 2d)의 경우, 구상인 알루미늄 사이에 CF(pitch)가 아크릴과 잘 교반되어 빽빽하게 잘 매워져있었고, 일부 CF(pitch) 입자는 수직방향으로 세워져서 빈 공간을 채우고 있었다.The aluminum metal powder (Fig. 2a) is in the form of a complete spherical shape and the particle size is 7 to 15 μm, and the copper (Fig. 2b) is in the form of 3 to 10 μm in a deformed form, and nickel (Fig. 2c) is 3 to It had a particle size of 18㎛ and did not have a spherical shape or a complete spherical shape as much as aluminum. In the case of the polymer composite composition of Example 3-3 (FIG. 2D), CF (pitch) was well agitated with acrylic between spherical aluminum, and it was tightly filled, and some CF (pitch) particles were erected in a vertical direction and thus empty. It was filling the space.

탄소소재를 적정 조성비 이하로 첨가하는 경우에는 입자 사이의 빈 공간을 채우지 못해 열전도 특성 향상에 한계가 있고, 적정 조성비 이상 첨가할 경우 빈공간은 적더라도 수직 방향으로 열전달 입자가 많아지기 때문에 열전도 특성이 떨어질 수 있다.If carbon material is added below the proper composition ratio, it is not possible to fill the empty spaces between particles, so there is a limit to the improvement of heat conduction characteristics.If added above the appropriate composition ratio, heat transfer characteristics are increased because the number of heat transfer particles in the vertical direction is increased even if the empty space is small. It can fall.

반면에 실시예 3-3(도 2d)처럼 자체적인 열전도 특성도 우수하고 완전한 구상인 알루미늄과 열전도 특성도 우수하며 구조적으로 구상인 입자와 사이에 잘 형성되는 CF(pitch)를 적절한 조성비로 혼합하였을 때, 5~6W/mK급의 고열전도 고분자 혼합조성물을 제조할 수 있었다. 완전한 구상을 가지고 있는 알루미늄이 구조적으로 다른 금속파우더에 비해서 우수한 수직방향 열전도 특성을 가지고 있고, CF(pitch)를 첨가에 의하여 완전한 구상인 알루미나 입자 사이사이에 공간이 잘 매워지면서, 판상형인 구조인 흑연에 비해 CF(pitch)가 수직 방향으로 전달되는 입자가 적기 때문에 열전도 특성이 가장 우수한 것을 확인하였다.On the other hand, as in Example 3-3 (Fig. 2d), the self-conducting properties were excellent, and the perfectly spherical aluminum and the thermal conductivity were excellent, and the structurally spherical particles and CF (pitch) well formed between were mixed at an appropriate composition ratio. At this time, it was possible to prepare a 5 ~ 6W / mK class high thermal conductivity polymer mixed composition. Aluminum, which has a perfectly spherical shape, has superior vertical heat conduction characteristics compared to other metal powders structurally, and by adding CF (pitch), the space between the completely spherical alumina particles is well filled, and the plate-shaped structure is graphite. Compared to that, it was confirmed that the heat conduction property was the best because there were fewer particles in which the pitch (CF) was transmitted in the vertical direction.

이러한 결과로부터, 알루미늄에 탄소소재를 아크릴 바인더 40 중량부 기준0.5~2중량부로 소량만 첨가할 경우, 탄소소재 자체의 우수한 열전도성도 효과를 나타내지만 구상인 알루미늄 입자사이의 공간을 유연한 선형으로 채우며 수평 방향 뿐만이 아니라 수직 방향 열전도 특성도 향상시키는 효과가 있으며, 특히, 알루미늄과 탄소소재를 포함하는 고분자 복합조성물에서 아크릴 바인더 40 중량부 기준 탄소소재의 함량이 1.8~2중량부 내외로 첨가될 때 가장 우수한 열전도 특성을 나타냄을 확인하였다.From these results, when only a small amount of 0.5 to 2 parts by weight of a carbon material is added to aluminum in an amount of 0.5 to 2 parts by weight based on 40 parts by weight of an acrylic binder, the carbon material itself exhibits excellent thermal conductivity effect, but fills the space between spherical aluminum particles in a flexible linear shape. It has the effect of improving not only the direction but also the heat conduction characteristics in the vertical direction.In particular, it is the most excellent when the content of a carbon material based on 40 parts by weight of an acrylic binder is added within 1.8 to 2 parts by weight in a polymer composite composition containing aluminum and carbon materials. It was confirmed that the thermal conductivity properties were shown.

이제까지 본 발명에 대하여 그 바람직한 실시예들을 중심으로 살펴보았다. 본 발명이 속하는 기술 분야에서 통상의 지식을 가진 자는 본 발명이 본 발명의 본질적인 특성에서 벗어나지 않는 범위에서 변형된 형태로 구현될 수 있음을 이해할 수 있을 것이다. 그러므로 개시된 실시예들은 한정적인 관점이 아니라 설명적인 관점에서 고려되어야 한다. 본 발명의 범위는 전술한 설명이 아니라 특허 청구범위에 나타나 있으며, 그와 동등한 범위 내에 있는 모든 차이점은 본 발명에 포함된 것으로 해석되어야 할 것이다.So far, the present invention has been looked at around its preferred embodiments. Those of ordinary skill in the art to which the present invention pertains will be able to understand that the present invention can be implemented in a modified form without departing from the essential characteristics of the present invention. Therefore, the disclosed embodiments should be considered from an illustrative point of view rather than a limiting point of view. The scope of the present invention is shown in the claims rather than the foregoing description, and all differences within the scope equivalent thereto should be construed as being included in the present invention.

Claims (13)

아크릴계 수지 40 중량부 기준;
열전도성 금속 필러로서 알루미늄 58 내지 58.2 중량부; 및
열전도성 탄소 필러로서 피치(Pitch)계 탄소섬유 1.8 내지 2 중량부;를 포함하는,
열전도성 고분자 복합 조성물.
Based on 40 parts by weight of an acrylic resin;
58 to 58.2 parts by weight of aluminum as a thermally conductive metal filler; And
Including, 1.8 to 2 parts by weight of pitch-based carbon fiber as a thermally conductive carbon filler,
Thermally conductive polymer composite composition.
삭제delete 삭제delete 삭제delete 삭제delete 제1항에 있어서,
상기 피치(Pitch)계 탄소섬유는 섬유단면 평균직경이 13-22㎛인 것을 특징으로 하는, 열전도성 고분자 복합 조성물.
The method of claim 1,
The pitch (Pitch)-based carbon fiber is characterized in that the average diameter of the fiber cross-section 13-22㎛, thermally conductive polymer composite composition.
삭제delete 삭제delete 삭제delete 삭제delete 제1항에 따른 열전도성 고분자 복합 조성물을 포함하는 열전도성 접착체.A thermally conductive adhesive comprising the thermally conductive polymer composite composition according to claim 1. 제1항에 따른 열전도성 고분자 복합 조성물을 포함하는 열전도성 필름.A thermally conductive film comprising the thermally conductive polymer composite composition according to claim 1. 제1항에 따른 열전도성 고분자 복합 조성물을 포함하는 열전도성 테이프.A thermally conductive tape comprising the thermally conductive polymer composite composition according to claim 1.
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JP2017035802A (en) * 2015-08-07 2017-02-16 昭和電工株式会社 Manufacturing method of insulation heat release sheet, insulation heat release sheet and heat spreader
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Publication number Priority date Publication date Assignee Title
KR20090037948A (en) * 2006-07-28 2009-04-16 데이진 가부시키가이샤 Heat conductive adhesive
KR20120077995A (en) * 2010-12-31 2012-07-10 제일모직주식회사 High thermal conductive resin composition including a milled pitch based carbon fiber
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