JP2010285569A - Thermoconductive resin material and production method thereof - Google Patents

Thermoconductive resin material and production method thereof Download PDF

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JP2010285569A
JP2010285569A JP2009141816A JP2009141816A JP2010285569A JP 2010285569 A JP2010285569 A JP 2010285569A JP 2009141816 A JP2009141816 A JP 2009141816A JP 2009141816 A JP2009141816 A JP 2009141816A JP 2010285569 A JP2010285569 A JP 2010285569A
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particles
resin material
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particle diameter
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Yoshiki Hayashida
芳樹 林田
Yoshiharu Yamamoto
義春 山本
Kenichi Ikeda
健一 池田
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Panasonic Corp
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Abstract

<P>PROBLEM TO BE SOLVED: To provide a thermoconductive resin material having high heat conductivity and easy to process, using a composite material provided by filling thermoconductive particles in an organic polymer resin at a high density without flocculation. <P>SOLUTION: As for the thermoconductive resin material 1 provided by filling the thermoconductive particles in the organic polymer resin 5, the thermoconductive particles are mixed particles 4 having different particle diameter distribution, the mixed particles 4 are composed of crude particles 2 having an average particle diameter of ≥100 μm but ≤500 μm and fine particles 3 having an average particle diameter less than that of the crude particles 2, and the ratio of the average particle diameter of the crude particles 2 to that of the fine particles 3 is ≥30/1 but ≤180/1. <P>COPYRIGHT: (C)2011,JPO&INPIT

Description

本発明は、有機材料中に高熱伝導性粒子を含有させて複合化した熱伝導性樹脂材料およびその製造方法に関するものである。   The present invention relates to a thermally conductive resin material obtained by combining high thermal conductivity particles in an organic material and a method for producing the same.

従来、放熱のための熱伝導性を有する材料としては、銅、アルミニウム、マグネシウム等の高熱伝導率金属が一般的である。しかしながら、金属には導電性があるため、電気絶縁性を確保するといった観点からは使用できる範囲が限られている。例えば、コンピュータ等の電子回路基板では配線間の絶縁を保つ必要があることから、放熱部材として金属を使用することが制限されている。   Conventionally, high thermal conductivity metals such as copper, aluminum, and magnesium are generally used as materials having thermal conductivity for heat dissipation. However, since metal has conductivity, the usable range is limited from the viewpoint of ensuring electrical insulation. For example, since it is necessary to maintain insulation between wirings in an electronic circuit board such as a computer, the use of metal as a heat radiating member is limited.

一方、金属以外の電気絶縁性と熱伝導性を有した材料としては、アルミナ、窒化アルミニウム、窒化ホウ素等のセラミック材料がある。しかし、これらの材料は、硬い固体であることと、融点が２０００℃以上と非常に高いといった理由から、プレス成形や射出成形が困難であるために任意の形状に加工することに制限がある。   On the other hand, ceramic materials such as alumina, aluminum nitride, and boron nitride are examples of materials having electrical insulation and thermal conductivity other than metal. However, because these materials are hard solids and have a very high melting point of 2000 ° C. or higher, it is difficult to perform press molding or injection molding, and therefore there are limitations on processing into arbitrary shapes.

また、小型軽量化が求められる電子機器では、放熱用のヒートシンクを設置するスペースも極めて小さく、回路基板やその他の電子部品の形状に合わせて任意の形状に加工できる熱伝導材料が求められている。   In addition, in electronic devices that are required to be reduced in size and weight, a space for installing a heat sink for heat dissipation is also extremely small, and a heat conductive material that can be processed into any shape according to the shape of a circuit board or other electronic components is required. .

近年になって、樹脂等の有機ポリマー（母材）中に無機微粒子を混合させて複合化することで、微粒子の持つ特異な物性と有機ポリマー樹脂の柔軟で容易な加工性とを併せ持つ微粒子複合化樹脂材料の技術が注目されている。例えば、アルミナ等の高い熱伝導率を有するセラミック粒子を有機ポリマー樹脂中に混合させて複合化することで、熱伝導率の低い樹脂材料を高い熱伝導性を有する樹脂材料とすることができる。このような複合化樹脂材料は、融点が低く、１００℃〜２００℃程度の低温度での射出、プレス成形などによる成形や、フィルム状に成形するなどの加工も容易である。   In recent years, fine particle composites that combine the unique physical properties of fine particles with the flexible and easy processability of organic polymer resins by mixing inorganic fine particles into organic polymers (base materials) such as resins. The technology of synthetic resin materials has attracted attention. For example, by mixing ceramic particles having a high thermal conductivity such as alumina into an organic polymer resin to form a composite, a resin material having a low thermal conductivity can be used as a resin material having a high thermal conductivity. Such a composite resin material has a low melting point, and can be easily processed by injection at a low temperature of about 100 ° C. to 200 ° C., molding by press molding, or molding into a film.

一方、このような複合化樹脂材料を放熱部材として利用するためには、樹脂材料中に充填する無機微粒子を高密度で充填して、複合化樹脂材料の熱伝導率を高めることが必要である。   On the other hand, in order to use such a composite resin material as a heat dissipation member, it is necessary to increase the thermal conductivity of the composite resin material by filling the resin material with inorganic fine particles at a high density. .

このような樹脂材料として、少なくとも０．２〜２μｍと２〜６３μｍの粒度分布領域に頻度ピークを有するアルミナ粉末を樹脂に配合した熱伝導性樹脂材料が特許文献１に開示されている。   As such a resin material, Patent Document 1 discloses a heat conductive resin material in which an alumina powder having a frequency peak in a particle size distribution region of at least 0.2 to 2 μm and 2 to 63 μm is blended with a resin.

また、粒子径５０〜３５０μｍの粒子を９０質量％以上含み、平均粒径が１００〜３００μｍの窒化ホウ素粉末と、平均粒径が１〜１０μｍの球状アルミナ粉末とからなる無機粉末を樹脂に含有させた熱伝導性樹脂材料が特許文献２に開示されている。   Further, the resin contains an inorganic powder composed of boron nitride powder having an average particle diameter of 100 to 300 μm and spherical alumina powder having an average particle diameter of 1 to 10 μm, containing 90% by mass or more of particles having a particle diameter of 50 to 350 μm. A thermally conductive resin material disclosed in Patent Document 2 is disclosed.

特開２００５−３０６７１８号公報JP-A-2005-306718 特開２００５−３４３９８３号公報JP 2005-343983 A

前述のように、有機ポリマー樹脂中に熱伝導性の無機粒子を混合させた微粒子複合化樹脂材料の熱伝導率を高めるためには、熱伝導率の高い無機微粒子を樹脂材料中に高密度で充填することが重要である。そのために、特許文献１に記載されているように複数の粒度ピークを持つ粒子を用い、大きな粒子の隙間を小さな粒子で埋めて、高密度に充填する方法が採られている。   As described above, in order to increase the thermal conductivity of the fine particle composite resin material in which the thermal conductive inorganic particles are mixed in the organic polymer resin, the inorganic fine particles having high thermal conductivity are added at a high density in the resin material. It is important to fill. Therefore, as described in Patent Document 1, a method is used in which particles having a plurality of particle size peaks are used, gaps between large particles are filled with small particles, and the particles are filled with high density.

しかしながら、アルミナや窒化アルミニウムなどの粒子は、単一粒子同士が凝集しやすい特性を有している。特に、粒子径が２μｍより小さくなると凝集が顕著となり、大きな粒子と小さな粒子とが均一に混じり合わずに、樹脂材料中での粒子の充填密度が不十分になるという問題があった。   However, particles such as alumina and aluminum nitride have a characteristic that single particles tend to aggregate. In particular, when the particle diameter is smaller than 2 μm, the aggregation becomes remarkable, and there is a problem that the packing density of the particles in the resin material becomes insufficient without uniformly mixing the large particles and the small particles.

粒子の充填密度が不十分であると、樹脂材料の熱伝導率が小さくなるため、発熱する回路基板の放熱部材としての適用することが困難となる。また、発熱部材の発熱量が大きい場合には、樹脂材料の温度が上昇して、樹脂材料自体が融解するなどの課題を有するものであった。   If the packing density of the particles is insufficient, the thermal conductivity of the resin material becomes small, making it difficult to apply as a heat dissipation member for a circuit board that generates heat. Further, when the heat generation amount of the heat generating member is large, the temperature of the resin material rises, and there is a problem that the resin material itself is melted.

本発明は、これらの課題を解決するためになされたもので、無機粒子を有機ポリマー樹脂中へ高密度に充填することで、高い熱伝導率を有し、かつ加工が容易で、ヒートシンクや放熱筐体等の用途に適した熱伝導性樹脂材料とその製造方法を提供することを目的とする。   The present invention has been made to solve these problems. By filling inorganic polymer particles in an organic polymer resin with high density, the present invention has high thermal conductivity and is easy to process, and can be used for heat sinks and heat dissipation. It aims at providing the heat conductive resin material suitable for uses, such as a housing | casing, and its manufacturing method.

上記目的を達成するために、本発明の熱伝導性樹脂材料は、熱伝導性粒子を有機ポリマー樹脂に充填した複合化材料からなる熱伝導性樹脂材料であって、熱導電性粒子は粒子径分布の異なる混合粒子であり、混合粒子は、１００μｍ以上５００μｍ以下の平均粒子径を有する第１粒子と、第１粒子よりも平均粒子径の小さな第２粒子とにより構成され、第１粒子の平均粒子径と第２粒子の平均粒子径との比が３０：１以上１８０：１以下である。   In order to achieve the above object, the thermally conductive resin material of the present invention is a thermally conductive resin material composed of a composite material in which thermally conductive particles are filled with an organic polymer resin, and the thermally conductive particles have a particle size of Mixed particles having different distributions, and the mixed particles are composed of first particles having an average particle diameter of 100 μm or more and 500 μm or less, and second particles having an average particle diameter smaller than the first particles, and the average of the first particles The ratio of the particle diameter to the average particle diameter of the second particles is 30: 1 or more and 180: 1 or less.

このような構成によれば、粒子径の大きな第１粒子の間に第２粒子を高密度で充填することが可能となり、樹脂材料中の混合粒子の充填密度を高めて、樹脂材料の熱伝導率を高めることができる。   According to such a configuration, the second particles can be filled at a high density between the first particles having a large particle diameter, and the packing density of the mixed particles in the resin material can be increased to increase the heat conduction of the resin material. The rate can be increased.

さらに、混合粒子の全体積に占める第２粒子の体積の割合が２０体積％以上５０体積％以下であることが好ましい。このような構成によれば、無機粒子の充填率をさらに増加させて、より熱伝導率の高い樹脂材料を実現することができる。   Furthermore, the volume ratio of the second particles in the total volume of the mixed particles is preferably 20% by volume or more and 50% by volume or less. According to such a configuration, it is possible to further increase the filling rate of the inorganic particles and realize a resin material with higher thermal conductivity.

さらに、第２粒子の平均粒子径が２μｍ以上であることが望ましい。このような構成によれば、第２粒子の凝集を抑制して、隣接する第１粒子の間隙により高密度に第２粒子を充填させてより高い熱伝導率を実現することが可能となる。   Furthermore, it is desirable that the average particle diameter of the second particles is 2 μm or more. According to such a configuration, it is possible to suppress the aggregation of the second particles and to fill the second particles at a high density with the gap between the adjacent first particles to realize a higher thermal conductivity.

さらに、導電性粒子が窒化アルミニウム粒子または炭化ケイ素粒子であることが好ましい。このような構成によれば、高い熱伝導率の樹脂材料を実現することができる。   Furthermore, the conductive particles are preferably aluminum nitride particles or silicon carbide particles. According to such a configuration, a resin material having high thermal conductivity can be realized.

さらに、第１粒子が炭化ケイ素粒子であり、第２粒子が窒化アルミニウム粒子であることが好ましい。このような構成によれば、さらに高い熱伝導率の樹脂材料を実現することができる。   Furthermore, it is preferable that the first particles are silicon carbide particles and the second particles are aluminum nitride particles. According to such a configuration, it is possible to realize a resin material having a higher thermal conductivity.

また、本発明の熱伝導性樹脂材料の製造方法は、１００μｍ以上５００μｍ以下の平均粒子径を有する第１粒子と、第１粒子の平均粒子径に対して１／１８０以上１／３０以下の平均粒子径を有する第２粒子との混合粒子を調合する工程と、加熱溶融した有機ポリマー樹脂に混合粒子を添加混合させて複合化樹脂材料を調製する工程と、複合化樹脂材料を所定の形状に加工する工程とを備える。   Moreover, the manufacturing method of the heat conductive resin material of this invention is the average of 1/180 or more and 1/30 or less with respect to the 1st particle | grains which have an average particle diameter of 100 micrometers or more and 500 micrometers or less, and the average particle diameter of 1st particle | grains. A step of preparing mixed particles with second particles having a particle size, a step of preparing a composite resin material by adding and mixing the mixed particles to a heated and melted organic polymer resin, and a composite resin material in a predetermined shape A processing step.

このような方法によれば、高い熱伝導率を有する混合粒子が高密度に充填されて高い熱伝導率を備え、なおかつ成型加工性に優れた熱伝導性樹脂材料を容易に実現することができる。   According to such a method, it is possible to easily realize a thermally conductive resin material having high thermal conductivity by being mixed with high density mixed particles having high thermal conductivity and having excellent moldability. .

また、本発明の熱伝導性樹脂材料の製造方法は、１００μｍ以上５００μｍ以下の平均粒子径を有する第１粒子と、第１粒子の平均粒子径に対して１／１８０以上１／３０以下の平均粒子径を有する第２粒子とを溶媒液に分散させて混合粒子分散溶媒液を調合する工程と、混合粒子分散溶媒液を有機ポリマー樹脂に添加混合させて複合化樹脂材料を調製する工程と、複合化樹脂材料を所定の形状に加工する工程とを備える。   Moreover, the manufacturing method of the heat conductive resin material of this invention is the average of 1/180 or more and 1/30 or less with respect to the 1st particle | grains which have an average particle diameter of 100 micrometers or more and 500 micrometers or less, and the average particle diameter of 1st particle | grains. A step of dispersing a second particle having a particle size in a solvent liquid to prepare a mixed particle dispersion solvent liquid, a step of adding a mixed particle dispersion solvent liquid to an organic polymer resin and preparing a composite resin material, And a step of processing the composite resin material into a predetermined shape.

このような方法によれば、高い熱伝導率を有する混合粒子が高密度に充填されて高い熱伝導率を備え、なおかつ成型加工性に優れた熱伝導性樹脂材料を容易に実現することができる。   According to such a method, it is possible to easily realize a thermally conductive resin material having high thermal conductivity by being mixed with high density mixed particles having high thermal conductivity and having excellent moldability. .

さらに、溶媒液が有機ポリマー樹脂を溶解可能であり、溶媒液が含まれる混合粒子分散溶媒液を有機ポリマー樹脂に添加混合させた後に、溶媒留去法により溶媒液を揮発飛散させて複合化樹脂材料を調製してもよい。このような方法によれば、より確実に混合粒子の分散が良好で溶媒の残留がない複合化樹脂材料を実現することができる。   Furthermore, the solvent liquid can dissolve the organic polymer resin, and after the mixed particle dispersion solvent liquid containing the solvent liquid is added to and mixed with the organic polymer resin, the solvent liquid is volatilized and scattered by a solvent distillation method to form a composite resin. Materials may be prepared. According to such a method, it is possible to realize a composite resin material that can more reliably disperse mixed particles and has no solvent remaining.

さらに、溶媒液が、トルエン、キシレン、シクロヘキサン、エタノールのいずれか１種または複数を含むことが望ましい。このような方法によれば、溶媒液中での特に粒子径の小さな無機粒子の凝集を抑制した分散が可能となり、粒子径の大きな無機粒子間に粒子径の小さな無機粒子を充填することが可能となる。   Furthermore, it is desirable that the solvent liquid contains one or more of toluene, xylene, cyclohexane, and ethanol. According to such a method, it is possible to disperse the inorganic particles having a small particle size in the solvent liquid while suppressing aggregation, and it is possible to fill the inorganic particles having a small particle size between the inorganic particles having a large particle size. It becomes.

さらに、第１粒子と第２粒子とが、窒化アルミニウム粒子または炭化ケイ素粒子であることが望ましい。このような方法によれば、さらに高い熱伝導率を有する樹脂材料を実現することができる。   Furthermore, it is desirable that the first particles and the second particles are aluminum nitride particles or silicon carbide particles. According to such a method, a resin material having a higher thermal conductivity can be realized.

以上のように本発明の熱伝導性樹脂材料およびその製造方法によれば、無機粒子同士の凝集を抑制して有機ポリマー樹脂中に高密度で充填した樹脂材料を実現することができ、高い熱伝導率を有した放熱部材などに好適な熱伝導性樹脂材料を実現することができる。   As described above, according to the thermally conductive resin material and the manufacturing method thereof of the present invention, it is possible to realize a resin material filled with high density in an organic polymer resin by suppressing aggregation of inorganic particles. A heat conductive resin material suitable for a heat radiating member having conductivity can be realized.

本発明の実施の形態１における熱伝導性樹脂材料の構成を示す概略図である。It is the schematic which shows the structure of the heat conductive resin material in Embodiment 1 of this invention. 同熱伝導性樹脂材料の製造方法を示すフローチャートである。It is a flowchart which shows the manufacturing method of the heat conductive resin material. 同熱伝導性樹脂材料に用いる窒化アルミニウムの粗粒子の粒子径分布を示す図である。It is a figure which shows the particle size distribution of the coarse particle of the aluminum nitride used for the heat conductive resin material. 同熱伝導性樹脂材料に用いる窒化アルミニウムの微粒子の粒子径分布を示す図である。It is a figure which shows the particle size distribution of the aluminum nitride microparticles | fine-particles used for the heat conductive resin material. 同熱伝導性樹脂材料における窒化アルミニウム粒子の微粒子混合率と混合粒子の充填密度との関係を示す図である。It is a figure which shows the relationship between the fine particle mixing rate of the aluminum nitride particle in the same heat conductive resin material, and the packing density of mixed particles. 同熱伝導性樹脂材料に用いる窒化アルミニウム粒子の粗粒子と微粒子の粒子径比と最大充填密度との関係を示す図である。It is a figure which shows the relationship between the particle diameter ratio of the coarse particle of aluminum nitride particle used for the heat conductive resin material, and microparticles | fine-particles, and the maximum packing density. 同熱伝導性樹脂材料に用いる窒化アルミニウム粒子の粗粒子の粒子径と最大充填密度との関係を示す図である。It is a figure which shows the relationship between the particle diameter of the coarse particle of the aluminum nitride particle used for the heat conductive resin material, and the maximum packing density. 同熱伝導性樹脂材料の熱伝導率を示す図である。It is a figure which shows the heat conductivity of the heat conductive resin material. 本発明の実施の形態２における熱伝導性樹脂材料の構成を示す概略図である。It is the schematic which shows the structure of the heat conductive resin material in Embodiment 2 of this invention. 同熱伝導性樹脂材料に用いる炭化ケイ素の粗粒子の粒子径分布を示す図である。It is a figure which shows the particle size distribution of the coarse particle of the silicon carbide used for the heat conductive resin material. 同熱伝導性樹脂材料に用いる窒化アルミニウムの微粒子の粒子径分布を示す図である。It is a figure which shows the particle size distribution of the aluminum nitride microparticles | fine-particles used for the heat conductive resin material. 同熱伝導性樹脂材料の熱伝導率を示す図である。It is a figure which shows the heat conductivity of the heat conductive resin material.

以下、本発明の実施の形態について、図面を用いて説明する。   Hereinafter, embodiments of the present invention will be described with reference to the drawings.

（実施の形態１）
本発明の実施の形態１における熱伝導性樹脂材料について図１〜図７を用いて説明する。 (Embodiment 1)
The heat conductive resin material in Embodiment 1 of this invention is demonstrated using FIGS.

図１は本発明の実施の形態１における熱伝導性樹脂材料の構成を示す概略図、図２は同熱伝導性樹脂材料の製造方法を示すフローチャート、図３Ａは同熱伝導性樹脂材料に用いる窒化アルミニウム（ＡｌＮ）の粗粒子の粒子径分布を示す図、図３Ｂは同熱伝導性樹脂材料に用いる窒化アルミニウム（ＡｌＮ）の微粒子の粒子径分布を示す図、図４は同熱伝導性樹脂材料における窒化アルミニウム（ＡｌＮ）粒子の微粒子混合率と混合粒子の充填密度との関係を示す図、図５は同熱伝導性樹脂材料に用いる窒化アルミニウム（ＡｌＮ）粒子の粗粒子と微粒子の粒子径比と最大充填密度との関係を示す図、図６は同熱伝導性樹脂材料に用いる窒化アルミニウム（ＡｌＮ）粒子の粗粒子の粒子径と最大充填密度との関係を示す図、図７は同熱伝導性樹脂材料の熱伝導率を示す図である。   FIG. 1 is a schematic diagram showing a configuration of a thermally conductive resin material in Embodiment 1 of the present invention, FIG. 2 is a flowchart showing a method for producing the thermally conductive resin material, and FIG. 3A is used for the thermally conductive resin material. FIG. 3B is a diagram showing the particle size distribution of aluminum nitride (AlN) coarse particles, FIG. 3B is a diagram showing the particle size distribution of aluminum nitride (AlN) particles used in the thermally conductive resin material, and FIG. 4 is the thermally conductive resin. The figure which shows the relationship between the fine particle mixing rate of the aluminum nitride (AlN) particle | grains in material, and the packing density of mixed particle | grains, FIG. 5 is the coarse particle of the aluminum nitride (AlN) particle | grain used for the heat conductive resin material, and the particle diameter of fine particle FIG. 6 is a diagram showing the relationship between the ratio and the maximum packing density, FIG. 6 is a diagram showing the relationship between the coarse particle size of the aluminum nitride (AlN) particles used in the thermally conductive resin material and the maximum packing density, and FIG. Thermal conductivity Is a diagram showing the thermal conductivity of the fat materials.

図１に示すように、本発明の実施の形態１における熱伝導性樹脂材料１は、第１粒子である窒化アルミニウム（ＡｌＮ）の粗粒子２の隙間に、第２粒子である窒化アルミニウム（ＡｌＮ）の微粒子３を充填させるようにした混合粒子４が、有機ポリマー樹脂５中に充填されて形成されている。   As shown in FIG. 1, the thermally conductive resin material 1 in Embodiment 1 of the present invention has aluminum nitride (AlN) as second particles in the gaps between coarse particles 2 of aluminum nitride (AlN) as first particles. The mixed particles 4 filled with the fine particles 3) are filled in the organic polymer resin 5 and formed.

すなわち、隣接する粗粒子２間の隙間に微粒子３が充填されるようにして窒化アルミニウム（ＡｌＮ）粒子の嵩密度を増加させ、有機ポリマー樹脂５中への窒化アルミニウム（ＡｌＮ）粒子の充填密度を増加させるようにしている。その結果、熱伝導性樹脂材料１中に占める熱伝導性の窒化アルミニウム（ＡｌＮ）粒子の割合が増加して、熱伝導性樹脂材料１の熱伝導率を高めることができ、成形が容易な放熱部材として使用可能な熱伝導性樹脂材料１を実現することが可能となる。   That is, the bulk density of the aluminum nitride (AlN) particles is increased so that the gaps between the adjacent coarse particles 2 are filled with the fine particles 3, and the packing density of the aluminum nitride (AlN) particles in the organic polymer resin 5 is increased. Try to increase. As a result, the proportion of thermally conductive aluminum nitride (AlN) particles in the thermally conductive resin material 1 is increased, the thermal conductivity of the thermally conductive resin material 1 can be increased, and heat dissipation is easy. It becomes possible to realize the thermally conductive resin material 1 that can be used as a member.

以下、本発明の実施の形態１における熱伝導性樹脂材料１の製造方法を、図２に示すフローチャートを用いて詳しく説明する。   Hereinafter, the manufacturing method of the heat conductive resin material 1 in Embodiment 1 of this invention is demonstrated in detail using the flowchart shown in FIG.

まず、図３Ａに示す粒子径分布を持った平均粒子径が３００μｍの窒化アルミニウム（ＡｌＮ）の粗粒子２を６０ｇと、図３Ｂに示す粒子径分布を持った平均粒子径が５μｍの窒化アルミニウム（ＡｌＮ）の微粒子３の４０ｇとをそれぞれ秤量して準備する（ステップＳ１０１、Ｓ１０２）。   First, 60 g of aluminum nitride (AlN) coarse particles 2 having an average particle size of 300 μm having the particle size distribution shown in FIG. 3A and aluminum nitride having an average particle size of 5 μm having a particle size distribution shown in FIG. 3B ( 40 g of fine particles 3 of AlN) are weighed and prepared (steps S101 and S102).

その後、両者を混合して粒子全体に占める微粒子３の比率が４０重量％となる窒化アルミニウム（ＡｌＮ）の混合粒子４を１００ｇ調合する（ステップＳ１０３）。   Thereafter, both are mixed to prepare 100 g of mixed particles 4 of aluminum nitride (AlN) in which the ratio of the fine particles 3 to the entire particles is 40% by weight (step S103).

続いて、軟化点９０℃、比重０．９２の有機ポリマー樹脂５を１２ｇ準備し、１９０℃の温度で加熱溶融して溶融有機ポリマー樹脂を準備する（ステップＳ１０４）。   Subsequently, 12 g of an organic polymer resin 5 having a softening point of 90 ° C. and a specific gravity of 0.92 is prepared, and heated and melted at a temperature of 190 ° C. to prepare a molten organic polymer resin (step S104).

この溶融有機ポリマー樹脂に、上述の窒化アルミニウム（ＡｌＮ）の混合粒子４の１００ｇを添加して、有機ポリマー樹脂５と、粗粒子２と微粒子３よりなる混合粒子４の窒化アルミニウム粒子との混合物を作製し、１９０℃の温度の下でこの混合物を３０分間攪拌する。この過程において、混合粒子４が有機ポリマー樹脂５に均一に混合した溶融混合物が調製される。次に、この溶融混合物を５０℃以下の温度になるまで冷却して固化させる。このようにして、平均粒子径が３００μｍの粗粒子２と平均粒子径が５μｍの微粒子３とからなる窒化アルミニウム（ＡｌＮ）粒子の混合粒子４の１００ｇが、有機ポリマー樹脂５の１２ｇの内部に均一に分布した熱伝導性樹脂材料１が作製される（ステップＳ１０５）。ここで作製された熱伝導性樹脂材料１中の混合粒子４の充填密度は、重量百分率では８９重量％となり、体積百分率に換算すると７０体積％となる。   100 g of the above-mentioned mixed particles 4 of aluminum nitride (AlN) is added to the molten organic polymer resin, and a mixture of the organic polymer resin 5 and the aluminum nitride particles of the mixed particles 4 composed of the coarse particles 2 and the fine particles 3 is added. Make and stir the mixture for 30 minutes at a temperature of 190 ° C. In this process, a molten mixture in which the mixed particles 4 are uniformly mixed with the organic polymer resin 5 is prepared. Next, this molten mixture is cooled to a temperature of 50 ° C. or lower and solidified. In this way, 100 g of mixed particles 4 of aluminum nitride (AlN) particles composed of coarse particles 2 having an average particle diameter of 300 μm and fine particles 3 having an average particle diameter of 5 μm are uniformly distributed within 12 g of organic polymer resin 5. The thermally conductive resin material 1 distributed in the above is produced (step S105). The packing density of the mixed particles 4 in the thermally conductive resin material 1 produced here is 89% by weight in terms of weight percentage, and 70% by volume in terms of volume percentage.

このように、粒子径分布の異なる混合粒子４を有機ポリマー樹脂５に混合して、微粒子３を粗粒子２の隙間に充填するようにすると、有機ポリマー樹脂５中に混合粒子４を高密度で充填することが可能となり、熱伝導率の高い熱伝導性樹脂材料１を作製することができる。   As described above, when the mixed particles 4 having different particle size distributions are mixed with the organic polymer resin 5 and the fine particles 3 are filled in the gaps of the coarse particles 2, the mixed particles 4 are densely packed in the organic polymer resin 5. It becomes possible to fill, and the heat conductive resin material 1 with high heat conductivity can be produced.

特に、本発明の実施の形態１では、混合粒子４は、１００μｍ以上５００μｍ以下の平均粒子径を有する第１粒子である粗粒子２と、第１粒子よりも平均粒子径の小さな第２粒子である微粒子３とにより構成され、粗粒子２の平均粒子径と微粒子３の平均粒子径との比が３０：１以上１８０：１以下となるようにしている。その結果、混合粒子４を調合する際の微粒子３の凝集が抑制されるとともに、微粒子３を隣接する粗粒子２の隙間に高密度に充填させることが可能となる。   In particular, in Embodiment 1 of the present invention, the mixed particles 4 are coarse particles 2 that are first particles having an average particle diameter of 100 μm or more and 500 μm or less, and second particles that are smaller in average particle diameter than the first particles. The ratio of the average particle diameter of the coarse particles 2 to the average particle diameter of the fine particles 3 is 30: 1 or more and 180: 1 or less. As a result, the aggregation of the fine particles 3 when preparing the mixed particles 4 is suppressed, and the fine particles 3 can be filled in the gaps between the adjacent coarse particles 2 with high density.

次に、このような熱伝導性樹脂材料１を、例えば射出成形やプレス成形などにより、放熱部材などに加工する（ステップＳ１０６）。   Next, the heat conductive resin material 1 is processed into a heat radiating member or the like by, for example, injection molding or press molding (step S106).

図４には、窒化アルミニウム（ＡｌＮ）の混合粒子４のうちの微粒子３の割合である微粒子混合率（体積％）に対する、熱伝導性樹脂材料１中の混合粒子４の充填率（体積％）を示し、粗粒子２と微粒子３との粒子径比（粗粒子平均粒子径／微粒子平均粒子径）をパラメータとして示している。   FIG. 4 shows the filling rate (volume%) of the mixed particles 4 in the thermally conductive resin material 1 with respect to the fine particle mixing ratio (volume%) which is the ratio of the fine particles 3 in the mixed particles 4 of aluminum nitride (AlN). The particle size ratio between the coarse particles 2 and the fine particles 3 (coarse particle average particle size / fine particle average particle size) is shown as a parameter.

図４から、例えば、粗粒子２の平均粒子径が３００μｍ、微粒子３の平均粒子径が５μｍで粒子径比が６０の混合粒子４では、微粒子３の微粒子混合率を４０体積％としたときに、最大充填密度７７体積％が得られる。また、粗粒子２の平均粒子径が３００μｍ、微粒子３の平均粒子径が３０μｍで粒子径比が１０の混合粒子４では、微粒子混合率を３０体積％としたときに最大充填密度７０体積％が得られる。さらに、粗粒子２の平均粒子径が３００μｍ、微粒子３の平均粒子径が３μｍで粒子径比が１００の混合粒子４では、微粒子混合率を４０体積％としたときに最大充填密度７９体積％が得られる。   From FIG. 4, for example, in the mixed particle 4 in which the average particle diameter of the coarse particles 2 is 300 μm, the average particle diameter of the fine particles 3 is 5 μm, and the particle diameter ratio is 60, the fine particle 3 mixing ratio is 40% by volume. A maximum packing density of 77% by volume is obtained. Further, in the mixed particles 4 in which the average particle size of the coarse particles 2 is 300 μm, the average particle size of the fine particles 3 is 30 μm, and the particle size ratio is 10, the maximum packing density is 70% by volume when the fine particle mixing rate is 30% by volume. can get. Furthermore, in the mixed particles 4 in which the average particle diameter of the coarse particles 2 is 300 μm, the average particle diameter of the fine particles 3 is 3 μm, and the particle diameter ratio is 100, the maximum packing density is 79 volume% when the fine particle mixing ratio is 40 volume%. can get.

図４の結果から、粗粒子２と微粒子３のいずれの粒子径比を有する混合粒子４でも、最大充填率となる微粒子３の混合率は２０体積％以上５０体積％以下の範囲に存在する。したがって、この範囲の中に、微粒子３の混合率を設定することによって熱伝導性樹脂材料１への熱伝導性粒子の充填率を大きくすることができ、より熱伝導性に優れた熱伝導性樹脂材料１を実現することができる。   From the results shown in FIG. 4, the mixing ratio of the fine particles 3 having the maximum filling rate is in the range of 20% by volume or more and 50% by volume or less in the mixed particles 4 having any particle size ratio of the coarse particles 2 and the fine particles 3. Therefore, by setting the mixing ratio of the fine particles 3 within this range, the filling rate of the heat conductive particles into the heat conductive resin material 1 can be increased, and the heat conductivity having a higher heat conductivity can be achieved. The resin material 1 can be realized.

また、図５には、第１粒子として平均粒子径３００μｍの窒化アルミニウム（ＡｌＮ）の粗粒子２を用い、混合粒子４に占める微粒子３の混合率を４０体積％とした熱伝導性樹脂材料１において、粗粒子２と微粒子３の粒子径比（粗粒子平均粒子径／微粒子平均粒子径）と最大充填密度の関係を示している。   Further, in FIG. 5, heat conductive resin material 1 in which coarse particles 2 of aluminum nitride (AlN) having an average particle diameter of 300 μm are used as the first particles and the mixing ratio of fine particles 3 in mixed particles 4 is 40 volume%. 2 shows the relationship between the particle size ratio between the coarse particles 2 and the fine particles 3 (coarse particle average particle size / fine particle average particle size) and the maximum packing density.

図５から、粗粒子２と微粒子３の粒子径比が３０以下になると、最大充填密度が急激に低下することがわかる。これは、微粒子３の粒子径が大きくなるか、または粗粒子２の粒子径が小さくなると、粗粒子２の隙間を微粒子３で埋めることができなくなるためである。   FIG. 5 shows that when the particle size ratio between the coarse particles 2 and the fine particles 3 is 30 or less, the maximum packing density rapidly decreases. This is because if the particle diameter of the fine particles 3 becomes large or the particle diameter of the coarse particles 2 becomes small, the gaps between the coarse particles 2 cannot be filled with the fine particles 3.

また、粒子径比が１５０以上となっても、最大充填密度は低下し、特に粒子径比が１８０以上で減少している。これは、粒子径比が１５０以上、すなわち微粒子３の平均粒子径が２μｍ以下となると、微粒子３が凝集して、粗粒子２と微粒子３とが均一に混じり合わなくなるためである。   Further, even when the particle size ratio is 150 or more, the maximum packing density is lowered, and in particular, the particle size ratio is reduced to 180 or more. This is because when the particle size ratio is 150 or more, that is, when the average particle size of the fine particles 3 is 2 μm or less, the fine particles 3 aggregate and the coarse particles 2 and the fine particles 3 are not mixed uniformly.

それ故に、混合粒子４における微粒子３の平均粒子径は、小さくとも２μｍ以上が望ましく、かつ、粗粒子２と微粒子３との粒子径比は３０以上１８０以下、望ましくは、５０以上１５０以下であれば熱伝導性樹脂材料１中に高密度に混合粒子４を充填させることができる。   Therefore, the average particle diameter of the fine particles 3 in the mixed particles 4 is desirably at least 2 μm, and the particle diameter ratio between the coarse particles 2 and the fine particles 3 is 30 or more and 180 or less, preferably 50 or more and 150 or less. For example, the mixed particles 4 can be filled in the heat conductive resin material 1 at a high density.

なお、上記の説明では、窒化アルミニウム（ＡｌＮ）の粗粒子２の平均粒子径を３００μｍとしたが、粗粒子２の平均粒子径によっても充填密度が異なる。   In the above description, the average particle diameter of the aluminum nitride (AlN) coarse particles 2 is set to 300 μm, but the packing density varies depending on the average particle diameter of the coarse particles 2.

図６には、粗粒子２と微粒子３の粒子径比を５０とし、混合粒子４全体に占める微粒子３の混合率を４０重量％とした熱伝導性樹脂材料１において、粗粒子２の平均粒子径を変えた場合の最大充填密度の変化を示している。   FIG. 6 shows the average particle size of the coarse particles 2 in the thermally conductive resin material 1 in which the particle diameter ratio between the coarse particles 2 and the fine particles 3 is 50 and the mixing ratio of the fine particles 3 in the mixed particles 4 is 40% by weight. The change of the maximum packing density when the diameter is changed is shown.

図６から、粗粒子２の平均粒子径が１００μｍ以下となると最大充填密度が低下することがわかる。これは、前述したように、粒子径比を５０として粗粒子２の平均粒子径を１００μｍとすると、微粒子３の粒子径が２μｍ以下となり微粒子３が凝集して、粗粒子２と均一に混じり合わなくなるためである。   FIG. 6 shows that the maximum packing density decreases when the average particle diameter of the coarse particles 2 is 100 μm or less. As described above, when the particle size ratio is 50 and the average particle size of the coarse particles 2 is 100 μm, the particle size of the fine particles 3 is 2 μm or less, and the fine particles 3 are aggregated and uniformly mixed with the coarse particles 2. This is because it disappears.

一方、粗粒子２の平均粒子径が５００μｍ以上になると、熱伝導性樹脂材料１の表面に窒化アルミニウム（ＡｌＮ）の粗粒子２が露出して凹凸が発生する。   On the other hand, when the average particle diameter of the coarse particles 2 is 500 μm or more, the coarse particles 2 of aluminum nitride (AlN) are exposed on the surface of the heat conductive resin material 1 to generate irregularities.

このような凹凸の発生は、熱伝導性樹脂材料１の表面の密着性を低下させるので、発熱部材と熱伝導性樹脂材料１との間の熱伝導性を低下させる。それ故に、窒化アルミニウムの粗粒子２の平均粒子径は５００μｍ以下とすることが好ましい。   The occurrence of such irregularities reduces the adhesion of the surface of the heat conductive resin material 1, and thus reduces the heat conductivity between the heat generating member and the heat conductive resin material 1. Therefore, the average particle diameter of the aluminum nitride coarse particles 2 is preferably 500 μm or less.

したがって、粒子の充填密度を向上させ、かつ熱伝導性樹脂材料の密着性を保つためには、窒化アルミニウム（ＡｌＮ）粗粒子２の平均粒子径が１００μｍ以上５００μｍ以下で、かつ粗粒子２と微粒子３との粒子径比は３０以上１８０以下であることが望ましい。   Therefore, in order to improve the packing density of the particles and maintain the adhesion of the heat conductive resin material, the average particle diameter of the aluminum nitride (AlN) coarse particles 2 is 100 μm or more and 500 μm or less, and the coarse particles 2 and the fine particles The particle size ratio with respect to 3 is preferably 30 or more and 180 or less.

次に、本発明の実施の形態１における熱伝導性樹脂材料１の熱伝導率について、図７を用いて説明する。   Next, the heat conductivity of the heat conductive resin material 1 in Embodiment 1 of this invention is demonstrated using FIG.

ここでは、熱伝導性樹脂材料１の熱伝導率を測定する試料片として、上述した製造方法に基づいて製造した熱伝導性樹脂材料１を温度１８０℃に加熱して再度溶融させて、プレス成形により直径１０ｍｍ、厚み３ｍｍの円盤状に加工し、その後冷却、固化して円盤状に形成した試料を用いている。   Here, as a sample piece for measuring the thermal conductivity of the thermal conductive resin material 1, the thermal conductive resin material 1 manufactured based on the above-described manufacturing method is heated to a temperature of 180 ° C. and melted again, and press molding is performed. Is used to prepare a sample that is processed into a disk shape having a diameter of 10 mm and a thickness of 3 mm, and then cooled and solidified to form a disk shape.

図７に、この試料片の熱伝導率をレーザーフラッシュ法により測定した結果を示し、比較例として粗粒子のみの窒化アルミニウム粒子で製造した場合、さらに、同じく比較例として有機ポリマー樹脂のみの熱伝導率を測定した結果を示している。   FIG. 7 shows the result of measurement of the thermal conductivity of this sample piece by the laser flash method. In the case where the sample is made of aluminum nitride particles having only coarse particles as a comparative example, the thermal conductivity of only an organic polymer resin is also used as a comparative example. The result of measuring the rate is shown.

図７において、サンプルＡは本発明の実施の形態１における熱伝導性樹脂材料、すなわち平均粒子径が３００μｍの粗粒子２と平均粒子径が５μｍの微粒子３とを充填密度４０体積％で混合した窒化アルミニウム（ＡｌＮ）粒子を用いた熱伝導性樹脂材料１の熱伝導率を示している。また、サンプルＢは図３Ａに示した平均粒子径３００μｍの窒化アルミニウム粒子のみの熱伝導性樹脂材料（充填密度４０体積％）を用いた場合の熱伝導率を示し、サンプルＣは有機ポリマー樹脂のみの熱伝導率を示している。   In FIG. 7, sample A is a heat conductive resin material according to Embodiment 1 of the present invention, that is, coarse particles 2 having an average particle diameter of 300 μm and fine particles 3 having an average particle diameter of 5 μm are mixed at a packing density of 40% by volume. The thermal conductivity of the thermally conductive resin material 1 using aluminum nitride (AlN) particles is shown. Sample B shows the thermal conductivity when only the aluminum nitride particles having an average particle diameter of 300 μm shown in FIG. 3A are used (packing density 40 vol%), and sample C is only organic polymer resin. The thermal conductivity of is shown.

図７から、サンプルＡの熱伝導率は８．２Ｗ／ｍ・Ｋであり、比較例としてのサンプルＢの熱伝導率の１．９Ｗ／ｍ・Ｋに比べて約４倍、サンプルＣの熱伝導率の０．４Ｗ／ｍ・Ｋに比べて約２０倍に向上していることがわかる。   From FIG. 7, the thermal conductivity of sample A is 8.2 W / m · K, which is about four times the thermal conductivity of sample B as a comparative example, 1.9 W / m · K. It can be seen that the conductivity is improved by about 20 times compared to 0.4 W / m · K.

以上説明したように、本実施の形態によれば、窒化アルミニウム（ＡｌＮ）の微粒子３の凝集を防止し、微粒子３と粗粒子２とを均一に混合することにより、粗粒子２間の隙間に微粒子３を高密度に充填することが可能となる。その結果、熱伝導性樹脂材料１内へ充填可能な最大充填密度が増加し、熱伝導性樹脂材料１内での熱伝導性粒子同士の接触面積が大きくなり、熱伝導性樹脂材料１として高い熱伝導率を実現することが可能となる。   As described above, according to the present embodiment, the aggregation of the aluminum nitride (AlN) fine particles 3 is prevented, and the fine particles 3 and the coarse particles 2 are uniformly mixed, so that the gaps between the coarse particles 2 are reduced. It becomes possible to fill the fine particles 3 with high density. As a result, the maximum packing density that can be filled into the heat conductive resin material 1 is increased, the contact area between the heat conductive particles in the heat conductive resin material 1 is increased, and the heat conductive resin material 1 is high. It becomes possible to realize thermal conductivity.

なお、本発明の実施の形態１における説明では、熱伝導性の粒子として窒化アルミニウム（ＡｌＮ）の粒子を用いたが、窒化アルミニウム（ＡｌＮ）に代えて炭化ケイ素（ＳｉＣ）の粒子を用いても同様の効果が得られる。   In the description of Embodiment 1 of the present invention, aluminum nitride (AlN) particles are used as thermally conductive particles, but silicon carbide (SiC) particles may be used instead of aluminum nitride (AlN). Similar effects can be obtained.

（実施の形態２）
本発明の実施の形態２における熱伝導性樹脂材料について図８〜図１０を用いて説明する。 (Embodiment 2)
The heat conductive resin material in Embodiment 2 of this invention is demonstrated using FIGS. 8-10.

図８は本発明の実施の形態２における熱伝導性樹脂材料の構成を示す概略図、図９Ａは同熱伝導性樹脂材料に用いる炭化ケイ素（ＳｉＣ）の粗粒子の粒子径分布を示す図、図９Ｂは同熱伝導性樹脂材料に用いる窒化アルミニウム（ＡｌＮ）の微粒子の粒子径分布を示す図、図１０は同熱伝導性樹脂材料の熱伝導率を示す図である。   FIG. 8 is a schematic diagram showing the configuration of the thermally conductive resin material in Embodiment 2 of the present invention, FIG. 9A is a diagram showing the particle size distribution of coarse particles of silicon carbide (SiC) used in the thermally conductive resin material, FIG. 9B is a view showing the particle size distribution of aluminum nitride (AlN) fine particles used for the thermally conductive resin material, and FIG. 10 is a view showing the thermal conductivity of the thermally conductive resin material.

図８に示すように、本発明の実施の形態２における熱伝導性樹脂材料１０は、第１粒子である粗粒子６として炭化ケイ素（ＳｉＣ）を用い、第２粒子である微粒子７として窒化アルミニウム（ＡｌＮ）を用いている。炭化ケイ素（ＳｉＣ）の粗粒子６の隙間に、窒化アルミニウム（ＡｌＮ）の微粒子７を充填させた混合粒子８を、有機ポリマー樹脂９の中に充填している。   As shown in FIG. 8, the thermally conductive resin material 10 in Embodiment 2 of the present invention uses silicon carbide (SiC) as the coarse particles 6 that are the first particles, and aluminum nitride as the fine particles 7 that are the second particles. (AlN) is used. Mixed particles 8 in which fine particles 7 of aluminum nitride (AlN) are filled in gaps between coarse particles 6 of silicon carbide (SiC) are filled in an organic polymer resin 9.

炭化ケイ素（ＳｉＣ）の粗粒子６の隙間に窒化アルミニウム（ＡｌＮ）の微粒子７が入り込むことにより、炭化ケイ素（ＳｉＣ）および窒化アルミニウム（ＡｌＮ）からなる熱伝導性粒子の混合粒子８の嵩密度が増加し、有機ポリマー樹脂９への充填密度を増加させることが可能となる。その結果、熱伝導性樹脂材料１０に占める熱伝導性の混合粒子８の割合が増加して、熱伝導性樹脂材料１０の熱伝導率を高めることができ、成形が容易な放熱部材として使用可能な熱伝導性樹脂材料１０を実現することが可能となる。   When the aluminum nitride (AlN) fine particles 7 enter the gaps between the silicon carbide (SiC) coarse particles 6, the bulk density of the mixed particles 8 of thermally conductive particles made of silicon carbide (SiC) and aluminum nitride (AlN) is reduced. It increases, and it becomes possible to increase the filling density to the organic polymer resin 9. As a result, the proportion of the thermally conductive mixed particles 8 in the thermally conductive resin material 10 increases, the thermal conductivity of the thermally conductive resin material 10 can be increased, and it can be used as a heat radiating member that can be easily molded. It is possible to realize a heat conductive resin material 10 that is stable.

本発明の実施の形態２における熱伝導性樹脂材料１０の製造方法は、基本的には本発明の実施の形態１における熱伝導性樹脂材料１の製造方法と同様であるので、図２に示すフローチャートを用いてその製造方法について詳しく説明する。   Since the manufacturing method of the heat conductive resin material 10 in Embodiment 2 of this invention is fundamentally the same as the manufacturing method of the heat conductive resin material 1 in Embodiment 1 of this invention, it shows in FIG. The manufacturing method will be described in detail using a flowchart.

まず、図９Ａに示すような粒子径分布を持った平均粒子径が３００μｍの炭化ケイ素（ＳｉＣ）の粗粒子６の６０ｇ（体積１８．６ｃｍ３に相当）と、図９Ｂに示す粒子径分布を持った平均粒子径が５μｍの窒化アルミニウム（ＡｌＮ）の微粒子７の４０ｇ（体積１２．３ｃｍ３に相当）とをそれぞれ秤量し、準備する（ステップＳ１０１、Ｓ１０２）。その後、両者を混合して全体に占める窒化アルミニウム（ＡｌＮ）の微粒子７の体積比率が４０体積％となる混合粒子８を１００ｇ（体積３０．９ｃｍ３に相当）調合する（ステップＳ１０３）。 First, 60 g (corresponding to a volume of 18.6 cm 3 ) of silicon carbide (SiC) coarse particles 6 having a particle size distribution as shown in FIG. 9A and an average particle size of 300 μm, and the particle size distribution shown in FIG. 40 g (corresponding to a volume of 12.3 cm 3 ) of the aluminum nitride (AlN) fine particles 7 having an average particle diameter of 5 μm are weighed and prepared (steps S101 and S102). Thereafter, both are mixed to prepare 100 g (corresponding to a volume of 30.9 cm 3 ) of mixed particles 8 in which the volume ratio of aluminum nitride (AlN) fine particles 7 occupying the whole is 40 volume% (step S103).

続いて、軟化点９０℃、比重０．９２の有機ポリマー樹脂９の１２ｇ（体積１３．０ｃｍ３に相当）を１９０℃の温度で加熱溶融して溶融有機ポリマー樹脂を準備する（ステップＳ１０４）。 Subsequently, 12 g (corresponding to a volume of 13.0 cm 3 ) of the organic polymer resin 9 having a softening point of 90 ° C. and a specific gravity of 0.92 is heated and melted at a temperature of 190 ° C. to prepare a molten organic polymer resin (step S104).

この溶融有機ポリマー樹脂に対し、上記の混合粒子８の１００ｇを添加して、有機ポリマー樹脂と混合粒子８とを混合させ、１９０℃の温度の下で３０分間ほど攪拌する。   100 g of the mixed particles 8 are added to the molten organic polymer resin, the organic polymer resin and the mixed particles 8 are mixed, and stirred at a temperature of 190 ° C. for about 30 minutes.

この工程によって、炭化ケイ素（ＳｉＣ）の粗粒子６と窒化アルミニウム（ＡｌＮ）の微粒子７の混合粒子８が均一に混合した有機ポリマー樹脂９の溶融混合物が調製される。   By this step, a molten mixture of organic polymer resin 9 in which mixed particles 8 of coarse particles 6 of silicon carbide (SiC) and fine particles 7 of aluminum nitride (AlN) are uniformly mixed is prepared.

次に、この溶融混合物を５０℃以下の温度になるまで冷却して固化させる。   Next, this molten mixture is cooled to a temperature of 50 ° C. or lower and solidified.

このようにして、平均粒子径が３００μｍの炭化ケイ素（ＳｉＣ）の粗粒子６と平均粒子径が５μｍの窒化アルミニウム（ＡｌＮ）の微粒子７とが混合された混合粒子８の１００ｇが、有機ポリマー樹脂９の１２ｇの内部に均一に分布した熱伝導性樹脂材料１０を作製できる（ステップＳ１０５）。   Thus, 100 g of the mixed particles 8 in which the coarse particles 6 of silicon carbide (SiC) having an average particle diameter of 300 μm and the fine particles 7 of aluminum nitride (AlN) having an average particle diameter of 5 μm are mixed together are organic polymer resins. 9 can be produced (step S105).

このとき、作製された熱伝導性樹脂材料１０中の混合粒子８の充填密度は、重量百分率では８９重量％となり、体積百分率に換算すると７０体積％となる。   At this time, the packing density of the mixed particles 8 in the produced thermally conductive resin material 10 is 89% by weight in terms of weight percentage, and 70% by volume in terms of volume percentage.

特に、本発明の実施の形態２では、混合粒子８は、１００μｍ以上５００μｍ以下の平均粒子径を有する粗粒子６と、粗粒子６よりも平均粒子径の小さな微粒子７とにより構成され、粗粒子６の平均粒子径と微粒子７の平均粒子径との比が３０：１以上１８０：１以下となるようにしている。その結果、混合粒子８を調合する際の微粒子７の凝集が抑制されるとともに、微粒子７を隣接する粗粒子６の隙間に高密度に充填させることが可能となる。   In particular, in Embodiment 2 of the present invention, the mixed particles 8 are composed of coarse particles 6 having an average particle diameter of 100 μm or more and 500 μm or less, and fine particles 7 having an average particle diameter smaller than the coarse particles 6, and the coarse particles The ratio of the average particle size of 6 to the average particle size of the fine particles 7 is set to be 30: 1 or more and 180: 1 or less. As a result, the aggregation of the fine particles 7 when the mixed particles 8 are prepared is suppressed, and the fine particles 7 can be filled in the gaps between the adjacent coarse particles 6 with high density.

次に、このような熱伝導性樹脂材料１０を、例えば射出成形やプレス成形などにより、放熱部材などに加工する（ステップＳ１０６）。   Next, the heat conductive resin material 10 is processed into a heat radiating member or the like by, for example, injection molding or press molding (step S106).

上述の実施の形態２における熱伝導性樹脂材料１０では、熱伝導性粒子の粗粒子６として窒化アルミニウム（ＡｌＮ）よりも熱伝導率が高い炭化ケイ素（ＳｉＣ）を使用しており、実施の形態１で説明した窒化アルミニウム（ＡｌＮ）粒子のみの場合と比べて、熱伝導率をさらに高くすることができる。   In the heat conductive resin material 10 in the above-described second embodiment, silicon carbide (SiC) having a higher thermal conductivity than aluminum nitride (AlN) is used as the coarse particles 6 of the heat conductive particles. Compared with the case of only the aluminum nitride (AlN) particles described in 1, the thermal conductivity can be further increased.

一般的に、炭化ケイ素（ＳｉＣ）は硬度が高いため、１０μｍ以下の粒子径に粉砕しにくい。このため、本発明の実施の形態２では微粒子７に窒化アルミニウム（ＡｌＮ）を用いて粗粒子６と微粒子７との混合による高密度充填を実現している。   Generally, since silicon carbide (SiC) has high hardness, it is difficult to grind to a particle size of 10 μm or less. For this reason, in Embodiment 2 of the present invention, high density filling is realized by mixing coarse particles 6 and fine particles 7 by using aluminum nitride (AlN) for fine particles 7.

次に、本発明の実施の形態２において作製した熱伝導性樹脂材料１０の熱伝導率について図１０を用いて説明する。   Next, the thermal conductivity of the thermally conductive resin material 10 produced in Embodiment 2 of the present invention will be described with reference to FIG.

ここでは、熱伝導性樹脂材料１０の熱伝導率を測定する試料片として、上述した製造方法に基づいて製造した熱伝導性樹脂材料１０を温度１８０℃に加熱して再度溶融させて、プレス成形により直径１０ｍｍ厚み３ｍｍの円盤状に加工し、その後冷却、固化して円盤状に形成した試料を用いている。   Here, as a sample piece for measuring the thermal conductivity of the thermally conductive resin material 10, the thermally conductive resin material 10 manufactured based on the above-described manufacturing method is heated to 180 ° C. and melted again, and press molding is performed. The sample which was processed into a disk shape with a diameter of 10 mm and a thickness of 3 mm, and then cooled and solidified to form a disk shape is used.

図１０には、本発明の実施の形態２における試料片の熱伝導率をレーザーフラッシュ法により測定した結果をサンプルＤとして示し、比較例として実施の形態１の窒化アルミニウム（ＡｌＮ）のみの混合粒子を用いた熱伝導性樹脂材料の熱伝導率をサンプルＥ、同じく比較例として炭化ケイ素（ＳｉＣ）の平均粒子径３００μｍの粗粒子のみを用いた熱伝導性樹脂材料の熱伝導率をサンプルＦとして示している。   In FIG. 10, the result of measuring the thermal conductivity of the sample piece in Embodiment 2 of the present invention by the laser flash method is shown as Sample D, and as a comparative example, mixed particles of only the aluminum nitride (AlN) of Embodiment 1 The thermal conductivity of the thermally conductive resin material using the sample is the sample E, and the thermal conductivity of the thermally conductive resin material using only coarse particles of silicon carbide (SiC) having an average particle diameter of 300 μm as the comparative example is the sample F. Show.

図１０から、本発明の実施の形態２における熱伝導性樹脂材料１０は、熱伝導率が１１．２Ｗ／ｍ・Ｋであり、比較例としての実施の形態１における熱伝導性樹脂材料１の熱伝導率の８．２Ｗ／ｍ・Ｋに比べて、約１．３倍に向上している。また、平均粒子径３００μｍの炭化ケイ素（ＳｉＣ）粒子のみの熱伝導性樹脂材料の熱伝導率の２．２Ｗ／ｍ・Ｋと比べると、約５倍に向上していることがわかる。   From FIG. 10, the heat conductive resin material 10 in the second embodiment of the present invention has a thermal conductivity of 11.2 W / m · K, and the heat conductive resin material 1 in the first embodiment as a comparative example. Compared to the thermal conductivity of 8.2 W / m · K, it is improved about 1.3 times. In addition, it can be seen that the thermal conductivity of the silicon resin (SiC) particles having an average particle diameter of 300 μm alone is improved by about 5 times compared with the thermal conductivity of 2.2 W / m · K.

以上説明したように、本発明の実施の形態２のような材料の異なる微粒子と粗粒子とを混合する場合でも、粗粒子間の隙間に微粒子が充填されて、熱伝導性樹脂材料内へ充填密度を高めて、熱伝導樹脂材料内での粒子同士の接触面積を大きくし、熱伝導率を向上させることができる。   As described above, even when mixing fine particles and coarse particles of different materials as in Embodiment 2 of the present invention, the fine particles are filled in the gaps between the coarse particles and filled into the thermally conductive resin material. It is possible to increase the density, increase the contact area between the particles in the heat conductive resin material, and improve the thermal conductivity.

なお、上述した実施の形態１、２では、図２に示した製造方法のフローチャートに従って、溶融した有機ポリマー樹脂に窒化アルミニウムまたは炭化ケイ素の粒子を添加混合させて、熱伝導性樹脂材料を作製した例を記載した。しかし、熱伝導性樹脂材料の製造方法は上記の方法に限定されることはない。   In the first and second embodiments described above, in accordance with the flowchart of the manufacturing method shown in FIG. 2, aluminum nitride or silicon carbide particles are added and mixed into the molten organic polymer resin to produce a heat conductive resin material. An example was given. However, the manufacturing method of a heat conductive resin material is not limited to said method.

例えば、有機ポリマー樹脂を溶解可能な溶媒中に、異なる粒子径分布を持つ熱伝導性粒子を分散させた溶媒分散液を添加調合し、この溶媒分散液を有機ポリマー樹脂中に添加して有機ポリマー樹脂を溶解させて有機ポリマー樹脂と熱伝導性粒子とを混合させた後に、溶媒を留去する方法も可能である。   For example, a solvent dispersion in which thermally conductive particles having different particle size distributions are dispersed in a solvent capable of dissolving the organic polymer resin is added and formulated, and the solvent dispersion is added to the organic polymer resin to form an organic polymer. A method of distilling off the solvent after dissolving the resin and mixing the organic polymer resin and the thermally conductive particles is also possible.

このとき、有機溶媒としてはトルエン、キシレン、シクロヘキサン、エタノール等を利用でき、これらの溶媒を単独または複数種で混合して用いてもよい。   At this time, toluene, xylene, cyclohexane, ethanol, or the like can be used as the organic solvent, and these solvents may be used alone or in combination.

また、有機ポリマー樹脂を溶解しない溶媒を用いる場合は、加熱溶融した有機ポリマー樹脂中に熱伝導性粒子の混合分散溶媒液を滴下して添加し、溶融状態で攪拌して有機ポリマー樹脂と熱伝導性粒子とを混合させることにより、異なる粒子径分布を持つ混合粒子が均一に分布した複合化放熱性樹脂材料を作製することもできる。   In addition, when using a solvent that does not dissolve the organic polymer resin, add the mixed dispersion solvent liquid of thermally conductive particles dropwise into the heated and melted organic polymer resin, and stir in the molten state to conduct heat with the organic polymer resin. By mixing the conductive particles, a composite heat-dissipating resin material in which mixed particles having different particle size distributions are uniformly distributed can be produced.

以上のように本発明の熱伝導性樹脂材料とその製造方法は、放熱を必要とする電子機器や電気回路に適用可能な高い熱伝導性を有する熱伝導性樹脂材料を実現し、射出成形などにより、様々な形状のヒートシンクや、放熱部材などへの利用が可能である。   As described above, the thermally conductive resin material and the manufacturing method thereof according to the present invention realizes a thermally conductive resin material having high thermal conductivity that can be applied to an electronic device or an electric circuit that requires heat dissipation, and injection molding. Therefore, it can be used for various shapes of heat sinks, heat radiating members, and the like.

１，１０ 熱伝導性樹脂材料
２，６ 粗粒子
３，７ 微粒子
４，８ 混合粒子
５，９ 有機ポリマー樹脂 1,10 Thermally conductive resin material 2,6 Coarse particles 3,7 Fine particles 4,8 Mixed particles 5,9 Organic polymer resin

Claims (11)

熱伝導性粒子を有機ポリマー樹脂に充填した熱伝導性樹脂材料であって、
前記熱伝導性粒子は粒子径分布の異なる混合粒子であり、前記混合粒子は、１００μｍ以上５００μｍ以下の平均粒子径を有する第１粒子と、前記第１粒子よりも平均粒子径の小さな第２粒子とにより構成され、前記第１粒子の平均粒子径と前記第２粒子の平均粒子径との比が３０：１以上１８０：１以下であることを特徴とする熱伝導性樹脂材料。 A thermally conductive resin material in which thermally conductive particles are filled in an organic polymer resin,
The thermally conductive particles are mixed particles having different particle size distributions. The mixed particles include first particles having an average particle size of 100 μm or more and 500 μm or less, and second particles having an average particle size smaller than that of the first particles. And a ratio of the average particle diameter of the first particles to the average particle diameter of the second particles is 30: 1 or more and 180: 1 or less. 前記混合粒子の全粒子の体積に対して、前記第２粒子の体積が２０体積％以上５０体積％以下であることを特徴とする請求項１に記載の熱伝導性樹脂材料。 2. The thermally conductive resin material according to claim 1, wherein the volume of the second particles is 20 volume% or more and 50 volume% or less with respect to the volume of all the particles of the mixed particles. 前記第２粒子の平均粒子径が２μｍ以上であることを特徴とする請求項１または請求項２に記載の熱伝導性樹脂材料。 The heat conductive resin material according to claim 1 or 2, wherein an average particle diameter of the second particles is 2 µm or more. 前記熱伝導性粒子が窒化アルミニウム粒子または炭化ケイ素粒子であることを特徴とする請求項１から請求項３のいずれか一項に記載の熱伝導性樹脂材料。 The thermally conductive resin material according to any one of claims 1 to 3, wherein the thermally conductive particles are aluminum nitride particles or silicon carbide particles. 前記第１粒子が炭化ケイ素粒子であり、前記第２粒子が窒化アルミニウム粒子であることを特徴とする請求項１から請求項４のいずれか一項に記載の熱伝導性樹脂材料。 The thermally conductive resin material according to any one of claims 1 to 4, wherein the first particles are silicon carbide particles, and the second particles are aluminum nitride particles. １００μｍ以上５００μｍ以下の平均粒子径を有する第１粒子と、前記第１粒子の平均粒子径に対して１／１８０以上１／３０以下の平均粒子径を有する第２粒子との混合粒子を調合する工程と、
加熱溶融した有機ポリマー樹脂に前記混合粒子を添加混合させて複合化樹脂材料を調製する工程と、
前記複合化樹脂材料を所定の形状に加工する工程と
を備えることを特徴とする熱伝導性樹脂材料の製造方法。 A mixed particle of first particles having an average particle diameter of 100 μm or more and 500 μm or less and second particles having an average particle diameter of 1/180 or more and 1/30 or less with respect to the average particle diameter of the first particles is prepared. Process,
A step of preparing a composite resin material by adding and mixing the mixed particles to a heated and melted organic polymer resin; and
And a step of processing the composite resin material into a predetermined shape. １００μｍ以上５００μｍ以下の平均粒子径を有する第１粒子と、前記第１粒子の平均粒子径に対して１／１８０以上１／３０以下の平均粒子径を有する第２粒子とを溶媒液に分散させて混合粒子分散溶媒液を調合する工程と、
前記混合粒子分散溶媒液を有機ポリマー樹脂に添加混合させて複合化樹脂材料を調製する工程と、
前記複合化樹脂材料を所定の形状に加工する工程と
を備えることを特徴とする熱伝導性樹脂材料の製造方法。 First particles having an average particle diameter of 100 μm or more and 500 μm or less and second particles having an average particle diameter of 1/180 or more and 1/30 or less of the average particle diameter of the first particles are dispersed in a solvent liquid. Preparing a mixed particle dispersion solvent liquid,
A step of preparing a composite resin material by adding and mixing the mixed particle dispersion solvent liquid to an organic polymer resin; and
And a step of processing the composite resin material into a predetermined shape. 前記溶媒液が前記有機ポリマー樹脂を溶解可能であり、前記溶媒液が含まれる前記混合粒子分散溶媒液を有機ポリマー樹脂に添加混合させた後に、溶媒留去法により前記溶媒液を揮発飛散させて前記複合化樹脂材料を調製することを特徴とする請求項７に記載の熱伝導性樹脂材料の製造方法。 The solvent liquid can dissolve the organic polymer resin, and after the mixed particle dispersion solvent liquid containing the solvent liquid is added to and mixed with the organic polymer resin, the solvent liquid is volatilized and scattered by a solvent distillation method. The method for producing a thermally conductive resin material according to claim 7, wherein the composite resin material is prepared. 加熱溶融した前記有機ポリマー樹脂に前記混合粒子分散溶媒液を添加して攪拌混合させて前記複合化樹脂材料を調製することを特徴とする請求項７に記載の熱伝導性樹脂材料の製造方法。 The method for producing a thermally conductive resin material according to claim 7, wherein the mixed resin material is prepared by adding the mixed particle-dispersed solvent liquid to the heat-melted organic polymer resin and stirring and mixing the mixture. 前記溶媒液が、トルエン、キシレン、シクロヘキサン、エタノールのいずれか１種または複数を含むことを特徴とする請求項８に記載の熱伝導性樹脂材料の製造方法。 The method for producing a thermally conductive resin material according to claim 8, wherein the solvent liquid contains one or more of toluene, xylene, cyclohexane, and ethanol. 前記第１粒子と前記第２粒子とが、窒化アルミニウム粒子または炭化ケイ素粒子であることを特徴とする請求項６から請求項１０のいずれか一項に記載の熱伝導性樹脂材料の製造方法。 The method for producing a thermally conductive resin material according to any one of claims 6 to 10, wherein the first particles and the second particles are aluminum nitride particles or silicon carbide particles.
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