JP2020176222A - Aluminum nitride composite filler - Google Patents
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Abstract
Description
本発明は、新規な窒化アルミニウムからなる複合フィラーを提供するものである。詳しくは、多面体粒子からなる窒化アルミニウム粉末と、窒化アルミニウムウィスカーが存在する新規な複合フィラーを提供するものである。 The present invention provides a novel composite filler made of aluminum nitride. Specifically, it provides an aluminum nitride powder composed of polyhedral particles and a novel composite filler in which an aluminum nitride whisker is present.
放熱シートや放熱グリースとして各種電子機器に広く利用される放熱材料として、シリコーンゴムやシリコーングリースに、熱伝導性フィラーを充填した組成物が使用されている。上記熱伝導性フィラーとして、電気絶縁性に優れており且つ高熱伝導性を有していることから、窒化アルミニウムが注目されている。 As a heat-dissipating material widely used in various electronic devices as a heat-dissipating sheet or heat-dissipating grease, a composition in which silicone rubber or silicone grease is filled with a thermally conductive filler is used. As the heat conductive filler, aluminum nitride has been attracting attention because it has excellent electrical insulation and high heat conductivity.
放熱材料の熱伝導率を向上させるには、高熱伝導性を有したフィラーを高充填することが重要であると考えられていた。そのため、放熱材料のフィラーとしての窒化アルミニウム粉末を構成する粒子としては、球状であり、数１０〜数１００μｍ程度の幅広い粒径分布とすることにより細密な充填構造を採ることが好ましいとされている（特許文献１参照）。 In order to improve the thermal conductivity of the heat-dissipating material, it was considered important to highly fill the filler with high thermal conductivity. Therefore, it is said that the particles constituting the aluminum nitride powder as the filler of the heat radiating material are spherical, and it is preferable to adopt a fine packing structure by having a wide particle size distribution of about several to several hundred μm. (See Patent Document 1).
一方、絶縁放熱用フィラーとして、細長い針状の形状をした窒化アルミニウムである窒化アルミニウムウィスカーが知られている（特許文献２参照）。この窒化アルミニウムウィスカーは、優れた電気絶縁性と高い熱伝導性を有しているが、樹脂中において窒化アルミニウムウィスカーがランダムな方向を向くように充填させる必要があり、充填方法、成形方法によりその性能にバラツキが発生することが懸念される。 On the other hand, an aluminum nitride whisker, which is an elongated needle-shaped aluminum nitride, is known as a filler for heat insulation and heat dissipation (see Patent Document 2). This aluminum nitride whisker has excellent electrical insulation and high thermal conductivity, but it is necessary to fill the aluminum nitride whisker in the resin so that it faces in a random direction, and depending on the filling method and molding method, the aluminum nitride whisker must be filled. There is concern that performance will vary.
このため、本発明者らは、窒化アルミニウム粉末と、窒化アルミニウムウィスカーとを組み合わせて放熱性を向上させようと試みた。一般に窒化アルミニウムウィスカーと組み合わせる窒化アルミニウム粉末としては、焼結顆粒のような大粒径の球状粒子が使用される。ウィスカーと大粒径粉球状粒子では、点接触で熱パス経路が構成される。 Therefore, the present inventors have attempted to improve heat dissipation by combining aluminum nitride powder and aluminum nitride whiskers. Generally, as the aluminum nitride powder to be combined with the aluminum nitride whiskers, spherical particles having a large particle size such as sintered granules are used. In whiskers and large particle size powder spherical particles, a thermal path path is constructed by point contact.
近年、材料自体の軽質化や高粘性樹脂・無溶媒樹脂の使用に伴い、それ自体の充填を少なくしても、放熱性などの効果を発揮しうる放熱性フィラーが望まれている。しかしながら、点接触では、熱パスが少ないため、低充填の場合の熱伝導性を高くできないという課題があった。 In recent years, as the material itself has become lighter and the highly viscous resin / solvent-free resin has been used, there has been a demand for a heat-dissipating filler that can exhibit effects such as heat-dissipating properties even if the filling of the material itself is reduced. However, in point contact, there is a problem that the thermal conductivity cannot be increased in the case of low filling because the heat path is small.
従って、本発明の目的は、樹脂に充填した際、従来のフィラー形状では達成できない優れた熱伝導性の付与を可能とした窒化アルミニウム複合フィラーを提供することにある。 Therefore, an object of the present invention is to provide an aluminum nitride composite filler capable of imparting excellent thermal conductivity that cannot be achieved by a conventional filler shape when filled in a resin.
そこで本発明者ら、上記課題についてさらに検討した結果、多面体粒子を含む窒化アルミニウム粉末と、窒化アルミニウムウィスカーとを組み合わせることで、接触面積が多くなり、熱パス経路が多くなるため、従来の球状粒子を用いる場合よりも、熱伝導性を高く担保することができ、低充填量で充填した樹脂に優れた熱伝導性を付与し得ることを見出し、本発明を完成するに至った。 Therefore, as a result of further study on the above problems, the present inventors further investigated, and as a result, by combining the aluminum nitride powder containing the polyhedron particles and the aluminum nitride whisker, the contact area is increased and the heat path path is increased, so that the conventional spherical particles It has been found that the thermal conductivity can be ensured higher than that in the case of using the above, and excellent thermal conductivity can be imparted to the resin filled with a low filling amount, and the present invention has been completed.
本発明の構成は以下の通りである。
すなわち本発明にかかる複合フィラーは、少なくとも２面の平坦面を有する面構造を備えた多面体粒子であり、粒度分布曲線における累積５０％値（Ｄ50）が２０μｍ〜２００μｍの窒化アルミニウム粉末と、平均直径（Ｄ）が０．１〜１．０μｍであり、平均長さ（Ｌ）が１０〜８０μｍの範囲にある窒化アルミニウムウィスカーとを含む。
複合フィラー中の、前記窒化アルミニウム粉末と、窒化アルミニウムウィスカーとの合計体積を１００体積％としたときに、窒化アルミニウム粉末を８０〜９０体積％、窒化アルミニウムウィスカーを２０〜１０体積％の比率で含むことが好ましい。
このような複合フィラーは、揮発性溶媒中に、窒化アルミニウム粉末と、窒化アルミニウムウィスカーを分散させたのち、噴霧乾燥することで製造することができる。
本発明の樹脂組成物は、前記複合フィラーと樹脂成分と、樹脂組成物の体積に対して、前記複合フィラーを５〜８０体積％で含む。
The configuration of the present invention is as follows.
That is, the composite filler according to the present invention is a polyhedral particle having a surface structure having at least two flat surfaces, and is an average of aluminum nitride powder having a cumulative 50% value (D 50 ) of 20 μm to 200 μm in the particle size distribution curve. It includes an aluminum nitride whisker having a diameter (D) of 0.1 to 1.0 μm and an average length (L) in the range of 10 to 80 μm.
When the total volume of the aluminum nitride powder and the aluminum nitride whisker in the composite filler is 100% by volume, the aluminum nitride powder is contained in a ratio of 80 to 90% by volume and the aluminum nitride whisker is contained in a ratio of 20 to 10% by volume. Is preferable.
Such a composite filler can be produced by dispersing aluminum nitride powder and aluminum nitride whiskers in a volatile solvent and then spray-drying the composite filler.
The resin composition of the present invention contains the composite filler, the resin component, and the composite filler in an amount of 5 to 80% by volume based on the volume of the resin composition.
本発明の複合フィラーは、所定の窒化アルミニウム粉末と窒化アルミニウムウィスカーとを組み合わせているので、ウィスカーの線状部分が多面体と線接触ないし面接触するため、熱パス経路が多くなり、従来の球状粒子を用いる場合よりも、熱伝導性を高く担保することができ、高粘性樹脂や無溶媒樹脂など、充填量を多くできない樹脂であっても、低充填量で充填した樹脂に優れた熱伝導性を付与できる。 Since the composite filler of the present invention is a combination of a predetermined aluminum nitride powder and aluminum nitride whisker, the linear portion of the whisker makes line contact or surface contact with the polyhedron, so that the number of heat path paths increases and the conventional spherical particles It is possible to secure higher thermal conductivity than the case of using, and even if the resin cannot be filled in a large amount such as a highly viscous resin or a solvent-free resin, the resin filled with a low filling amount has excellent thermal conductivity. Can be granted.
以下、本発明の実施形態を説明するが、本発明はこれらの記載に何ら限定されない。 Hereinafter, embodiments of the present invention will be described, but the present invention is not limited to these descriptions.
＜窒化アルミニウム粉末＞
窒化アルミニウム粉末は、少なくとも２面の平坦面を有する面構造を備えた多面体粒子であり、粒度分布曲線における累積５０％値（Ｄ50）が２０μｍ〜２００μｍ、好ましくは３０μｍ〜１００μｍの範囲にある。
<Aluminum nitride powder>
The aluminum nitride powder is a polyhedral particle having a surface structure having at least two flat surfaces, and the cumulative 50% value (D 50 ) in the particle size distribution curve is in the range of 20 μm to 200 μm, preferably 30 μm to 100 μm.
２面以上の平坦面があれば、粉末自体の形状は特に制限されず、たとえば、板状、円筒状、直方体状のように２面が平行で存在していてもよく、また四面体以上の多面体であってもよい。そのうち、四面体以上の多面体の面構造を有するものが、後述の窒化アルミニウムウィスカーと上記面との接触機会が多く、好適である。 As long as there are two or more flat surfaces, the shape of the powder itself is not particularly limited, and the two surfaces may exist in parallel, for example, a plate shape, a cylindrical shape, or a rectangular parallelepiped shape, or a tetrahedron or more. It may be a polyhedron. Among them, those having a polyhedral surface structure of tetrahedron or more are suitable because they have many opportunities for contact between the aluminum nitride whiskers described later and the above surface.
本発明で使用される多面体粒子は、ＳＥＭ写真による観察において、その特徴を確認することができる。例えば、図２は、本発明で使用される代表的な窒化アルミニウム粒子のＳＥＭ写真であり、上記図２において確認されるように、多面体形状を有し、複数の平面がランダムに存在する。さらに、国際公開2017/131239号にある、図３に示されるように、胴部の一部に六角柱形状を示すものも例示される。図３の粒子は、端部に椀状の凸部とを有する形状を成した窒化アルミニウム粒子である。完全な六角柱も本発明の態様に含まれ、六角柱の少なくとも一部の平面が維持される範囲で、角部が曲面もしくは平面に面取りされた形状、また、胴部の一部にくびれや出っ張りを有する形状であってもよい。 The characteristics of the polyhedral particles used in the present invention can be confirmed by observation with SEM photographs. For example, FIG. 2 is an SEM photograph of typical aluminum nitride particles used in the present invention, which has a polyhedral shape and has a plurality of planes randomly present, as confirmed in FIG. Furthermore, as shown in FIG. 3, which is published in International Publication No. 2017/131239, a hexagonal column shape is also exemplified in a part of the body. The particles in FIG. 3 are aluminum nitride particles having a shape having bowl-shaped protrusions at the ends. A complete hexagonal column is also included in the embodiment of the present invention, in which the corners are curved or chamfered to a flat surface as long as at least a part of the flat surface of the hexagonal column is maintained, and a part of the body is constricted. It may have a shape having a bulge.
窒化アルミニウム粉末は、該長径（Ｌ）に対する短径（Ｄ）との比（Ｌ／Ｄ）が０．８〜１．２であり、上記平面の少なくとも一面は、その面積（Ｓ）が、Ｓ／Ｌ≧１．０を満たすことが好ましい。 The aluminum nitride powder has a ratio (L / D) of the major axis (L) to the minor axis (D) of 0.8 to 1.2, and the area (S) of at least one surface of the plane is S. It is preferable that / L ≧ 1.0 is satisfied.
上記窒化アルミニウム粒子の表面を形成する平面は、窒化アルミニウムの結晶面に由来するものと考えられる。前記平面は、同方位の結晶面により構成される。上記平面は状態でランダムに存在する。 The plane forming the surface of the aluminum nitride particles is considered to be derived from the crystal plane of aluminum nitride. The plane is composed of crystal planes having the same orientation. The plane exists randomly in the state.
また、上記結晶面は、少なくとも１つの面、好ましくは、前記ＳＥＭ写真で観察される粒子の面積に対して、５０％以上、特に、８０％以上の面積比で存在し、その結晶面の面積（Ｓ）が、Ｓ／Ｌ≧１．０を満たす平面であると、上記窒化アルミニウム粉末には大面積を有する平面がランダムに存在するため、後述する窒化アルミニウムウィスカーとの間の接触面積が増加し、熱伝導率が向上した複合フィラーを得ることができる。
尚、上記面積比は、前記ＳＥＭ写真で観察される状態を画像解析により算出した値である。
Further, the crystal plane exists at least one plane, preferably in an area ratio of 50% or more, particularly 80% or more, with respect to the area of the particles observed in the SEM photograph, and the area of the crystal plane. When (S) is a plane satisfying S / L ≧ 1.0, the aluminum nitride powder has a plane having a large area at random, so that the contact area with the aluminum nitride whisker described later increases. Therefore, a composite filler having improved thermal conductivity can be obtained.
The area ratio is a value calculated by image analysis of the state observed in the SEM photograph.
＜窒化アルミニウムウィスカー＞
窒化アルミニウムウィスカーは、平均直径（Ｄ）が０．１〜１．０μｍ、好ましくは０．２〜０．９μｍであり、平均長さ（Ｌ）が１０〜８０μｍ、好ましくは１５〜７５μｍの範囲にある。
また、（Ｌ／Ｄ）は、１０〜８００、好ましくは１００〜７００である。
<Aluminum nitride whisker>
The aluminum nitride whiskers have an average diameter (D) of 0.1 to 1.0 μm, preferably 0.2 to 0.9 μm, and an average length (L) of 10 to 80 μm, preferably 15 to 75 μm. is there.
Further, (L / D) is 10 to 800, preferably 100 to 700.
このような窒化アルミニウムウィスカーを用いることにより、樹脂中において上記窒化アルミニウムウィスカーが上記窒化アルミニウム粉末に接触することで上記窒化アルミニウム粉末同士の橋渡しとして機能する。 By using such an aluminum nitride whisker, the aluminum nitride whisker comes into contact with the aluminum nitride powder in the resin and functions as a bridge between the aluminum nitride powders.
このような窒化アルミニウムウィスカーは、特開2017-149624号公報に記載の製造方法で、アルミナ粉末、カーボン粉末、遷移金属成分、及び硫黄成分を含む原料混合物を、上記遷移金属成分が、上記アルミナ粉末１００重量部に対して、元素換算で０．０５〜５重量部、上記硫黄成分が、上記遷移金属成分に対して、１０〜１０００ｍｏｌ％の割合となるように調整し、窒素雰囲気にて加熱して上記アルミナ粉末を還元窒化することで製造可能である。 Such an aluminum nitride whisker is produced by a production method described in JP-A-2017-149624, in which a raw material mixture containing an alumina powder, a carbon powder, a transition metal component, and a sulfur component is used, and the transition metal component is the alumina powder. Adjust so that the ratio of the sulfur component to the transition metal component is 10 to 1000 mol% with respect to 100 parts by weight in terms of elements of 0.05 to 5 parts, and heat the mixture in a nitrogen atmosphere. It can be produced by reducing and nitriding the above alumina powder.
また、前記窒化アルミニウムウィスカーの形状は、棒状であってもよいし、不規則に湾曲した線状であってもよい。
窒化アルミニウムウィスカーは、樹脂内で絡み合って構成される。ウィスカー同士が焼結したり融合して一体化しているものではなく、通常、ウィスカーは独立して存在しているが、一部が融合していたり焼結したりするものを除外するものではない。
Further, the shape of the aluminum nitride whiskers may be a rod shape or an irregularly curved linear shape.
Aluminum nitride whiskers are constructed intertwined within the resin. Whiskers are not sintered or fused and integrated, and whiskers usually exist independently, but do not exclude those that are partially fused or sintered. ..
＜複合フィラー＞
本発明にかかる複合フィラーは、前記窒化アルミニウム粉末と、窒化アルミニウムウィスカーとを含む。
各成分比はその効果を発揮できれば限定されないが、前記複合フィラー中の、前記窒化アルミニウム粉末と、窒化アルミニウムウィスカーとの合計体積を１００体積％としたときに、窒化アルミニウム粉末を８０〜９０体積％、窒化アルミニウムウィスカーを２０〜１０体積％の比率で含むことが好ましい。尚、前記窒化アルミニウム粉末及びウィスカーの割合は、対象とするフィラーの任意の箇所よりサンプリングした試料のＳＥＭ写真の視野範囲における面積割合（％）を体積％として示した値である。
<Composite filler>
The composite filler according to the present invention includes the aluminum nitride powder and the aluminum nitride whiskers.
Each component ratio is not limited as long as the effect can be exhibited, but when the total volume of the aluminum nitride powder and the aluminum nitride whisker in the composite filler is 100% by volume, the aluminum nitride powder is 80 to 90% by volume. , Aluminum nitride whisker is preferably contained in a ratio of 20 to 10% by volume. The ratio of the aluminum nitride powder and the whiskers is a value showing the area ratio (%) in the visual field range of the SEM photograph of the sample sampled from an arbitrary portion of the target filler as a volume%.
このような窒化アルミニウム粉末と窒化アルミニウムウィスカーとを組み合わせると、例えば図１（a）に示されるように、ウィスカーの線状部分が多面体構造の平面とが、線接触ないし面接触すると考えられる。このため、熱パス経路が多くなるため、熱伝導性を高く担保できると本発明者らは考えている。一方、球状粒子の場合、図１(b)に示されるようにウィスカーとの接触は点接触となり、熱パス経路が少なくなると考えられる。 When such an aluminum nitride powder and an aluminum nitride whisker are combined, for example, as shown in FIG. 1A, it is considered that the linear portion of the whisker is in line contact or surface contact with the plane of the polyhedral structure. For this reason, the present inventors consider that high thermal conductivity can be ensured because the number of heat path paths increases. On the other hand, in the case of spherical particles, as shown in FIG. 1 (b), the contact with the whiskers is a point contact, and it is considered that the number of heat path paths is reduced.
熱パス経路が多いと、充填した樹脂に対して優れた熱伝導性を付与できる。このため、低充填量であっても高い熱伝導性を付与できる上に、ウィスカーを含むことで、窒化アルミニウム粉末の沈降を抑制することもできる。 When there are many heat path paths, excellent thermal conductivity can be imparted to the filled resin. Therefore, high thermal conductivity can be imparted even with a low filling amount, and the inclusion of whiskers can suppress the sedimentation of the aluminum nitride powder.
複合フィラーの体積を１００体積％としたときに、窒化アルミニウム粉末および窒化アルミニウムウィスカーが占める割合が、７０体積％以上、好ましくは８０体積％以上、さらに好ましくは９０体積％以上であることが好ましい。 When the volume of the composite filler is 100% by volume, the ratio of the aluminum nitride powder and the aluminum nitride whiskers is preferably 70% by volume or more, preferably 80% by volume or more, and more preferably 90% by volume or more.
複合フィラーの体積に含まれる他の成分としては、空隙や他の充填材などが挙げられる。他の充填材として、具体的には、アルミナ粉末、窒化硼素粉末、ダイヤモンド粉末などを使用してもよい。これらを含むことで、樹脂成形体の熱伝導性の向上効果をより顕著に発揮できる場合がある。
複合フィラーは、所望の形状に賦形してもよく、例えば顆粒状であっても、シート形状であってもいずれでもよい。
Other components included in the volume of the composite filler include voids and other fillers. Specifically, as the other filler, alumina powder, boron nitride powder, diamond powder and the like may be used. By including these, the effect of improving the thermal conductivity of the resin molded product may be exhibited more remarkably.
The composite filler may be shaped into a desired shape, for example, either in the form of granules or in the form of a sheet.
複合フィラーの製造方法
本発明にかかる複合フィラーの製造方法は特に制限されず、窒化アルミニウムウィスカーと窒化アルミニウム粉末を公知の方法で混合すれば製造することが可能である。
たとえば、乾燥状態で、双方をブレンドすることで製造することが可能である。
Method for Producing Composite Filler The method for producing the composite filler according to the present invention is not particularly limited, and the composite filler can be produced by mixing aluminum nitride whiskers and aluminum nitride powder by a known method.
For example, it can be produced by blending both in a dry state.
また、揮発性溶媒中に、所定の割合で窒化アルミニウムウィスカーと窒化アルミニウム粉末を混合し、混合物スラリーを、噴霧乾燥させることで製造することができる。
さらに窒化アルミニウムウィスカーと窒化アルミニウム粉末を必要に応じてバインダーなどの存在下に混合し、混合物を、非せん断条件あるいは弱いせん断条件下に押出成形したのち、成形物を所定の形状に、加工することで製造することができる。なお強いせん断条件で押出成形すると、ウィスカーが切れたり、繊維と粒子の接触効率が低くなることがある。
いずれの製造方法でも分散媒としては、揮発性であれば特に制限されず、水、アセトン、アルコール、トルエン、エタノールなどを使用可能である。
Further, it can be produced by mixing aluminum nitride whiskers and aluminum nitride powder in a predetermined ratio in a volatile solvent and spray-drying the mixture slurry.
Further, the aluminum nitride whisker and the aluminum nitride powder are mixed in the presence of a binder or the like as necessary, the mixture is extruded under non-shearing conditions or weak shearing conditions, and then the molded product is processed into a predetermined shape. Can be manufactured at. If extrusion molding is performed under strong shear conditions, the whiskers may break or the contact efficiency between the fibers and the particles may decrease.
In any of the production methods, the dispersion medium is not particularly limited as long as it is volatile, and water, acetone, alcohol, toluene, ethanol and the like can be used.
＜樹脂組成物＞
本発明にかかる樹脂組成物は、上記複合フィラーとともに、樹脂成分とを含む。
樹脂成分はエポキシ樹脂、フェノール樹脂等の熱硬化性樹脂や、ポリエチレン、ポリプロピレン、ポリアミド、ポリカーボネート、ポリイミド、ポリフェニレンサルファルド等の熱可塑性樹脂、アクリル樹脂またシリコーンゴム、ＥＰＲ、ＳＢＲ等のゴム類、シリコーンオイル等が挙げられる。
<Resin composition>
The resin composition according to the present invention contains a resin component together with the above-mentioned composite filler.
The resin components are thermosetting resins such as epoxy resin and phenol resin, thermoplastic resins such as polyethylene, polypropylene, polyamide, polycarbonate, polyimide and polyphenylene sulfide, acrylic resin, silicone rubber, rubbers such as EPR and SBR, and silicone. Examples include oil.
さらに高粘性樹脂であっても充填が可能である。たとえばエポキシ、シリコーン、ポリイミド、ウレタン、アクリルから選ばれる少なくとも１種の樹脂成分と組み合わせることが好ましい。また、無溶媒樹脂は一般的に粘度が高いが、本発明の複合フィラーは、無溶媒の樹脂成分であっても、充填可能であり、無溶剤であると溶媒除去に伴う処理を省略できるという効果も奏する。 Further, even a highly viscous resin can be filled. For example, it is preferable to combine it with at least one resin component selected from epoxy, silicone, polyimide, urethane, and acrylic. Further, although the solvent-free resin generally has a high viscosity, the composite filler of the present invention can be filled even with a solvent-free resin component, and if it is solvent-free, the treatment associated with solvent removal can be omitted. It also has an effect.
樹脂組成物は、小さいシェアで混合して成形するか、或いは複合構造体を型に充填した後、上記液状の樹脂成分を含浸させ、上記樹脂を硬化させて成形体を得る方法が推奨される。なおメルトフローレートの高い熱可塑性樹脂に配合して混練し、成形することも可能である。 The recommended method is to mix and mold the resin composition with a small share, or to fill the mold with the composite structure, impregnate the liquid resin component, and cure the resin to obtain a molded product. .. It is also possible to mix it with a thermoplastic resin having a high melt flow rate, knead it, and mold it.
上記樹脂組成物において、複合フィラーの配合量は、特に制限されるものではないが、５〜８０体積％、好ましくは１０〜７５体積％が一般的である。充填量は、樹脂組成物の体積と複合構造体の体積から算出できる。
以上のような本発明にかかる複合フィラーは、優れた熱伝導性の付与を可能とした窒化アルミニウムからなる新たな材料を提供することが可能である。
In the above resin composition, the blending amount of the composite filler is not particularly limited, but is generally 5 to 80% by volume, preferably 10 to 75% by volume. The filling amount can be calculated from the volume of the resin composition and the volume of the composite structure.
The composite filler according to the present invention as described above can provide a new material made of aluminum nitride that can impart excellent thermal conductivity.
以下、本発明を実施例により、詳しく説明するが、本発明はこれらの実施例に何ら限定されるものではない。 Hereinafter, the present invention will be described in detail with reference to Examples, but the present invention is not limited to these Examples.
実施例および比較例で使用した窒化アルミニウム粒子は以下のようにして調製した。 The aluminum nitride particles used in Examples and Comparative Examples were prepared as follows.
製造例１：多面体窒化アルミニウム粒子
・アルミナ粉末
α−アルミナ：Ｄ50 ３．５１８μｍ
・カーボン粉末
カーボン粉末Ｂ：平均粒径 ２０ｎｍ、ＤＢＰ吸収量 １１５ｃｍ3／１００ｇ、含有
硫黄量 ３０００ｐｐｍ
・硫黄成分
硫黄粉末：純度 ９８％以上
Production Example 1: Polyhedral aluminum nitride particles / alumina powder α-alumina: D 50 3.518 μm
Carbon powder carbon powder B: average particle diameter 20 nm, DBP absorption 115cm 3 / 100g, content amount of sulfur 3000ppm
・ Sulfur component Sulfur powder: Purity 98% or more
以上の原材料を使用して、アルミナ粉末１００重量部及びカーボン粉末５０重量部からなる混合物に、該混合物内の硫黄成分量が上記アルミナ粉末１００重量部に対し５重量部となるように硫黄粉末を添加し、これらが均一に混合されるまで振動式攪拌機により混合し、原料混合物を得た。 Using the above raw materials, a sulfur powder is added to a mixture consisting of 100 parts by weight of alumina powder and 50 parts by weight of carbon powder so that the amount of sulfur components in the mixture is 5 parts by weight with respect to 100 parts by weight of the alumina powder. They were added and mixed with a vibrating stirrer until they were uniformly mixed to give a raw material mixture.
上記原料混合物を、カーボン製のセッターに、２０ｍｍ厚となるように収納し、窒素を流通可能な反応容器内にセットし、窒素ガスを流通させながら、加熱温度１７７５℃で還元窒化を行った。 The raw material mixture was stored in a carbon setter so as to have a thickness of 20 mm, nitrogen was set in a flowable reaction vessel, and reduction nitriding was performed at a heating temperature of 1775 ° C. while flowing nitrogen gas.
その際、反応容器に供給する一酸化炭素ガスの割合が５３体積％となるように、調整し、還元窒化反応を行い、還元窒化反応終了後、前記加熱温度を維持したまま、５時間保持して、反応容器より反応生成物を取り出した。 At that time, the ratio of carbon monoxide gas supplied to the reaction vessel is adjusted to 53% by volume, the reduction nitriding reaction is carried out, and after the reduction nitriding reaction is completed, the heating temperature is maintained for 5 hours. The reaction product was taken out from the reaction vessel.
その後、上記反応生成物を、大気雰囲気において７００℃で、５時間加熱して未反応のカーボン粉末を燃焼除去し、窒化アルミニウム粉末を得た。上記方法により得られた窒化アルミニウム粒子は、図２に示されるような多面体粒子で、Ｄ50 ３0μｍであった。窒化アルミニウム粒子を任意に１０粒選択して、前記測定方法に従い、長径（Ｌ）、短径粒（Ｄ）を測定したところ、Ｌ／Ｄは1.02であった。また、ＳＥＭ写真をもとに該粒子表面に存在する平面の面積（Ｓ）がＳ／Ｌ≧１．０を満たす面について、窒化アルミニウム粒子全表面に対する割合は３０％であった。 Then, the reaction product was heated at 700 ° C. for 5 hours in an air atmosphere to burn off the unreacted carbon powder to obtain an aluminum nitride powder. The aluminum nitride particles obtained by the above method were polyhedral particles as shown in FIG. 2, and had a D 50 of 30 μm. When 10 aluminum nitride particles were arbitrarily selected and the major axis (L) and minor axis particles (D) were measured according to the above measurement method, the L / D was 1.02. Further, based on the SEM photograph, the ratio of the area (S) of the plane existing on the particle surface to the entire surface of the aluminum nitride particles was 30% with respect to the surface satisfying S / L ≧ 1.0.
製造例２：球状窒化アルミニウム粒子
窒化アルミニウム粉末に焼結助剤として酸化イットリウム、有機結合剤及び溶媒を添加混合しスラリーを作製後、スプレードライヤーで得られた約３０μｍ球状造粒粉を得た。球状造粒粉を１００℃で乾燥後、５００℃の酸素雰囲気下で有機結合剤を燃焼除去したのち、１７５０℃で焼結し、焼結顆粒よりなる窒化アルミニウム粉末を製造した。
Production Example 2: Spherical aluminum nitride particles Yttrium oxide, an organic binder and a solvent were added and mixed with aluminum nitride powder as a sintering aid to prepare a slurry, and then a approximately 30 μm spherical granulated powder obtained by a spray dryer was obtained. The spherical granulated powder was dried at 100 ° C., the organic binder was burnt and removed in an oxygen atmosphere at 500 ° C., and then sintered at 1750 ° C. to produce an aluminum nitride powder composed of sintered granules.
実施例１
平均直径０．５μｍ、平均長さ６０μｍからなる窒化アルミニウム繊維；１５体積％、製造例１の多面体窒化アルミニウム粒子を含む窒化アルミニウム粉末；８５体積％混合物からなる窒化アルミニウム複合フィラーを用意した。
Example 1
An aluminum nitride fiber having an average diameter of 0.5 μm and an average length of 60 μm; an aluminum nitride powder containing 15% by volume and polyhedral aluminum nitride particles of Production Example 1; an aluminum nitride composite filler composed of an 85% by volume mixture was prepared.
得られた複合フィラーと、エポキシ樹脂とを羽根型撹拌機にて撹拌して、厚さ１ｍｍの樹脂組成物を作製した。具体的には樹脂としてエポキシ樹脂（三菱化学株式会社ｊＥＲ８２８）１００重量部と硬化剤（イミダゾール系硬化剤、四国化成工業株式会社製キュアゾール２Ｅ４ＭＺ）５重量部との混合物を、基材樹脂として準備した。次に、基材樹脂と、複合フィラーとを、複合フィラーの充填率が６０体積％となるように羽根型撹拌機にて混合して樹脂組成物を作製した。 The obtained composite filler and the epoxy resin were stirred with a blade-type stirrer to prepare a resin composition having a thickness of 1 mm. Specifically, a mixture of 100 parts by weight of an epoxy resin (Mitsubishi Chemical Co., Ltd. jER828) and 5 parts by weight of a curing agent (imidazole-based curing agent, Curesol 2E4MZ manufactured by Shikoku Kasei Kogyo Co., Ltd.) was prepared as a base resin. .. Next, the base resin and the composite filler were mixed with a vane-type stirrer so that the filling ratio of the composite filler was 60% by volume to prepare a resin composition.
得られた樹脂組成物の一部を金型体に注型し、熱プレスを使用し、温度：１００℃、圧力：１０ＭＰａ、保持時間：２時間の条件で硬化させ、直径１０ｍｍ、厚さ１ｍｍの樹脂組成物を得た。 A part of the obtained resin composition was cast into a mold and cured by using a hot press under the conditions of temperature: 100 ° C., pressure: 10 MPa, holding time: 2 hours, and the diameter was 10 mm and the thickness was 1 mm. Resin composition of.
得られた樹脂組成物の熱伝導率測定は、レーザーフラッシュ法熱物性測定装置（京都電子製ＬＦＡ−５０２）を用いて実施した。熱伝導率を測定した結果、実施例１の複合フィラーを用いた場合は７．０Ｗ／ｍＫであった。 The thermal conductivity of the obtained resin composition was measured using a laser flash method thermophysical property measuring device (LFA-502 manufactured by Kyoto Electronics Co., Ltd.). As a result of measuring the thermal conductivity, it was 7.0 W / mK when the composite filler of Example 1 was used.
実施例２
実施例１において、複合フィラーを、充填率が７０体積％となるように基体樹脂と混合した以外は実施例１と同様にして、樹脂組成物を作製した。
得られた樹脂組成物の熱伝導率は８．１Ｗ／ｍＫであった。
Example 2
In Example 1, a resin composition was prepared in the same manner as in Example 1 except that the composite filler was mixed with the substrate resin so that the filling rate was 70% by volume.
The thermal conductivity of the obtained resin composition was 8.1 W / mK.
比較例１
多面体窒化アルミニウム粒子の代わりに、製造例２の球状窒化アルミニウム粒子を使用した以外は、同様にして複合フィラーを調製した。複合フィラーと、エポキシ樹脂とを、複合フィラーの充填率が６０体積％となるように実施例１と同様に混合して樹脂組成物を作製した。
得られた樹脂組成物の熱伝導率は６．５Ｗ／ｍＫであった。
Comparative Example 1
A composite filler was prepared in the same manner except that the spherical aluminum nitride particles of Production Example 2 were used instead of the polyhedral aluminum nitride particles. A resin composition was prepared by mixing the composite filler and the epoxy resin in the same manner as in Example 1 so that the filling ratio of the composite filler was 60% by volume.
The thermal conductivity of the obtained resin composition was 6.5 W / mK.
比較例２
比較例１において、複合フィラーを、充填率が７０体積％となるように基体樹脂と混合した以外は比較例１と同様にして、樹脂組成物を作製した。
得られた樹脂組成物の熱伝導率は７．３Ｗ／ｍＫであった。
Comparative Example 2
In Comparative Example 1, a resin composition was prepared in the same manner as in Comparative Example 1 except that the composite filler was mixed with the substrate resin so that the filling rate was 70% by volume.
The thermal conductivity of the obtained resin composition was 7.3 W / mK.
以上の結果から、多面体窒化アルミニウム粒子を使用すると、同じ複合フィラーの充填率にしたときに、球状窒化アルミニウム粒子を使用する場合に比べて、ウィスカーとの接触面が多くなり、高熱伝導率を組成物に付与できることが分かった。 From the above results, when polyhedral aluminum nitride particles are used, the number of contact surfaces with whiskers increases when the filling rate of the same composite filler is used, and high thermal conductivity is composed as compared with the case where spherical aluminum nitride particles are used. It turned out that it can be given to things.
Claims (4)
平均直径（Ｄ）が０．１〜１．０μｍであり、平均長さ（Ｌ）が１０〜８０μｍの範囲にある窒化アルミニウムウィスカーとを含む、複合フィラー。 Aluminum nitride powder having a surface structure having at least two flat surfaces and having a cumulative 50% value (D 50 ) of 20 μm to 200 μm in the particle size distribution curve.
A composite filler comprising an aluminum nitride whiskers having an average diameter (D) of 0.1 to 1.0 μm and an average length (L) in the range of 10 to 80 μm.
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| WO2023149472A1 (en) * | 2022-02-04 | 2023-08-10 | 国立大学法人東海国立大学機構 | Resin molded product and method for producing same |
| WO2024048600A1 (en) * | 2022-08-30 | 2024-03-07 | 株式会社トクヤマ | Aluminum nitride powder and resin composition |
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