JP2005281346A - Phase change heat-conductive molding - Google Patents

Phase change heat-conductive molding Download PDF

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JP2005281346A
JP2005281346A JP2004093636A JP2004093636A JP2005281346A JP 2005281346 A JP2005281346 A JP 2005281346A JP 2004093636 A JP2004093636 A JP 2004093636A JP 2004093636 A JP2004093636 A JP 2004093636A JP 2005281346 A JP2005281346 A JP 2005281346A
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heat conductive
phase change
molded body
electronic component
plasticizer
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JP4511858B2 (en
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Hiroyuki Fujisawa
洋之 藤澤
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Polymatech Co Ltd
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Polymatech Co Ltd
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Abstract

<P>PROBLEM TO BE SOLVED: To obtain a phase change heat-conductive molding, which has excellent heat conduction performance and readily increases handleability and transfer properties. <P>SOLUTION: The phase change heat-conductive molding is obtained by molding a phase change heat-conductive composition, comprising a styrene-based elastomer, paraffin oil, a heat-conductive filler and a plasticizer having 40-60°C freezing point. The plasticizer in an amount of 50-400 parts wt. is added to the styrene-based elastomer in an amount of 100 parts wt. The plasticizer is preferably triphenyl phosphate. The phase change heat-conductive filler has a sheetlike form and is set to 50-300 μm thickness at <40°C. <P>COPYRIGHT: (C)2006,JPO&NCIPI

Description

本発明は、電子機器内における発熱電子部品と放熱器等の冷却部材との間に介在されて、発熱電子部品から冷却部材への熱伝導を促進する相変化熱伝導性成形体に関するものである。   The present invention relates to a phase change heat conductive molded body that is interposed between a heat generating electronic component in an electronic device and a cooling member such as a radiator and promotes heat conduction from the heat generating electronic component to the cooling member. .

近年、コンピュータのCPU(中央処理装置)を代表とする電子部品の高性能化に伴い、電子部品の消費電力及び発熱量は増大している。電子部品は熱により処理能力が低下する。よって、電子部品の性能を維持するために電子部品の蓄熱を回避する必要があり、電子部品の冷却が重要な課題となっている。このため、電子部品と冷却部材との間に介在される相変化熱伝導性成形体には、優れた熱伝導性能が求められている。   In recent years, power consumption and heat generation of electronic components have increased with the improvement in performance of electronic components typified by computer CPUs (central processing units). The processing capacity of electronic components is reduced by heat. Therefore, it is necessary to avoid heat storage of the electronic component in order to maintain the performance of the electronic component, and cooling of the electronic component is an important issue. For this reason, the phase change thermal conductive molded body interposed between the electronic component and the cooling member is required to have excellent thermal conductivity.

従来、この種の相変化熱伝導性成形体としては、ポリオレフィンと、金属粉末等の熱伝導性充填材とを含有する組成物からなるものが知られている(例えば、特許文献1参照。)。この相変化熱伝導性成形体は、ポリオレフィンの分子構造を適宜変更することにより、相変化温度が電子部品の使用温度範囲と一致するように設定されている。この相変化熱伝導性成形体は、前記電子部品の使用温度範囲内で相変化(可塑化)して電子部品と冷却部材との両方に密着し、それらの界面における接触熱抵抗値(界面接触熱抵抗値)を低下させて熱伝導性能を高める。   Conventionally, as this type of phase change heat conductive molded body, one made of a composition containing polyolefin and a heat conductive filler such as metal powder is known (for example, see Patent Document 1). . This phase change heat conductive molding is set so that the phase change temperature matches the operating temperature range of the electronic component by appropriately changing the molecular structure of the polyolefin. This phase change thermally conductive molded body undergoes phase change (plasticization) within the operating temperature range of the electronic component, and is in close contact with both the electronic component and the cooling member, and the contact thermal resistance value at the interface (interface contact) The thermal conductivity is improved by reducing the thermal resistance value.

また、相変化熱伝導性成形体として、スチレン系エラストマーと、パラフィンオイルと、熱伝導性充填材とを含有する組成物から成形されているものもある(例えば、特許文献2〜6参照。)。パラフィンオイルは、配合量の増加に伴い相変化熱伝導性成形体の相変化温度を低下させる。このため、パラフィンオイルの配合量を増加させることにより、相変化温度が前記電子部品の使用温度範囲と一致するように設定されている。この相変化熱伝導性成形体は、パラフィンオイルの配合量を調節することにより相変化温度を調整できるため、分子構造の変更を必要とする特許文献1に記載の相変化熱伝導性成形体に比べて相変化温度の調整が容易である。
特開2002−121332号公報 特開2003−113318号公報 特開2003−113272号公報 特開2003−82245号公報 特開2003−82244号公報 特開2003−49046号公報
Moreover, as a phase change heat conductive molded object, what is shape | molded from the composition containing a styrene-type elastomer, paraffin oil, and a heat conductive filler (for example, refer patent documents 2-6). . Paraffin oil lowers the phase change temperature of the phase change heat conductive molded body as the blending amount increases. For this reason, the phase change temperature is set to coincide with the operating temperature range of the electronic component by increasing the blending amount of paraffin oil. Since this phase change heat conductive molded body can adjust the phase change temperature by adjusting the blending amount of paraffin oil, the phase change heat conductive molded body described in Patent Document 1 that requires a change in molecular structure is used. In comparison, the phase change temperature can be easily adjusted.
JP 2002-121332 A JP 2003-133318 A JP 2003-113272 A JP 2003-82245 A JP 2003-82244 A JP 2003-49046 A

ところが、特許文献2〜6に記載の相変化熱伝導性成形体では、相変化温度が前記電子部品の使用温度範囲と一致するまでパラフィンオイルを増量すると、強度が低下して千切れ易くなるとともに硬度が低下して潰れ易くなり、さらに粘着性が過剰に高くなる。よって、この相変化熱伝導性成形体は、低強度で千切れ易いために、取扱い性(ハンドリング性)が低く、かつ低硬度で電子部品への取付け時(転写時)に加えられる荷重により潰れ易く、さらには粘着性が過剰に高いために電子部品への転写が困難であるという問題があった。   However, in the phase change heat conductive moldings described in Patent Documents 2 to 6, when the amount of paraffin oil is increased until the phase change temperature matches the operating temperature range of the electronic component, the strength is reduced and it is easily cut off. Hardness is reduced and it becomes easy to be crushed, and the adhesiveness becomes excessively high. Therefore, since this phase change heat conductive molded body is low in strength and easy to tear, it has low handleability (handling property) and low hardness, and it is crushed by a load applied during mounting to electronic parts (during transfer). In addition, there is a problem that transfer to an electronic component is difficult due to excessively high adhesiveness.

本発明は、このような従来技術に存在する問題点に着目してなされたものである。その目的とするところは、熱伝導性能に優れるとともにハンドリング性及び転写性を高めることが容易な相変化熱伝導性成形体を提供することにある。   The present invention has been made paying attention to such problems existing in the prior art. An object of the present invention is to provide a phase change heat conductive molded body that is excellent in heat conduction performance and easy to improve handling and transferability.

上記の目的を達成するために、請求項1に記載の発明の相変化熱伝導性成形体は、スチレン系エラストマーと、パラフィンオイルと、熱伝導性充填材と、凝固点が40〜60℃の範囲内である可塑剤とを含有する相変化熱伝導性組成物により成形されているものである。   In order to achieve the above object, the phase change heat conductive molded body of the invention according to claim 1 is a styrenic elastomer, paraffin oil, a heat conductive filler, and a freezing point in the range of 40 to 60 ° C. It is molded by a phase change heat conductive composition containing a plasticizer.

請求項2に記載の発明の相変化熱伝導性成形体は、スチレン系エラストマーと、パラフィンオイルと、熱伝導性充填材と、トリフェニルホスフェートからなる可塑剤とを含有する相変化熱伝導性組成物により成形されているものである。   The phase change heat conductive molded body of the invention according to claim 2 is a phase change heat conductive composition containing a styrene elastomer, paraffin oil, a heat conductive filler, and a plasticizer comprising triphenyl phosphate. It is molded by a product.

請求項3に記載の発明の相変化熱伝導性成形体は、請求項1又は請求項2に記載の発明において、前記可塑剤は、スチレン系エラストマー100重量部に対し50〜400重量部の割合で含有されているものである。   The phase change heat conductive molded body of the invention described in claim 3 is the invention according to claim 1 or claim 2, wherein the plasticizer is a ratio of 50 to 400 parts by weight with respect to 100 parts by weight of the styrene elastomer. It is contained in.

請求項1から請求項3に記載の発明の相変化熱伝導性成形体は、相変化熱伝導性組成物中に凝固点が40〜60℃の範囲内である可塑剤が含有されているために、40℃未満の常温での強度が高められるとともに取扱いや転写に適した硬度及び粘着性を有する。さらに、相変化熱伝導性成形体の温度が可塑剤の凝固点を超える温度に達すると、相変化熱伝導性成形体の可塑化が引き起こされて界面接触熱抵抗値が低下する。このため、相変化熱伝導性成形体は、熱伝導性能に優れるとともにハンドリング性及び転写性を高めることが容易である。   Since the phase change heat conductive molded object of the invention according to claims 1 to 3 contains a plasticizer having a freezing point in the range of 40 to 60 ° C. in the phase change heat conductive composition. In addition, the strength at room temperature of less than 40 ° C. can be increased, and the hardness and adhesiveness suitable for handling and transfer can be obtained. Furthermore, when the temperature of the phase change thermally conductive molded body reaches a temperature exceeding the freezing point of the plasticizer, plasticization of the phase change thermally conductive molded body is caused and the interfacial contact thermal resistance value decreases. For this reason, the phase change heat conductive molded body is excellent in heat conduction performance and easy to improve handling and transferability.

請求項4に記載の発明の相変化熱伝導性成形体は、請求項1から請求項3のいずれか一項に記載の発明において、シート状をなし、40℃未満のときの厚みが50〜300μmに設定されているものである。   The phase change heat conductive molded body of the invention according to claim 4 is the sheet according to any one of claims 1 to 3, and has a sheet shape and a thickness of 50 to less than 40 ° C. It is set to 300 μm.

従って、請求項4に記載の発明の相変化熱伝導性成形体は、40℃未満のときの厚みを前記範囲に設定することにより、40℃未満の常温での強度を高めてハンドリング性を高めるとともに、熱抵抗値を低下させて熱伝導性能を高めることができる。   Therefore, the phase change heat conductive molded body of the invention described in claim 4 has a strength at a room temperature of less than 40 ° C. and a handling property by setting the thickness when the temperature is less than 40 ° C. to the above range. At the same time, the thermal resistance can be lowered to increase the heat conduction performance.

請求項5に記載の発明の相変化熱伝導性成形体は、請求項1から請求項4のいずれか一項に記載の発明において、40〜80℃の温度範囲内で相変化を引き起こすものである。
従って、請求項5に記載の発明の相変化熱伝導性成形体は、電子部品の使用温度範囲内で電子部品に密着するように相変化し、界面接触熱抵抗値を低下させて熱伝導性能を高めることができる。
The phase change heat conductive molded body of the invention according to claim 5 causes phase change in the temperature range of 40 to 80 ° C. in the invention according to any one of claims 1 to 4. is there.
Therefore, the phase change heat conductive molded body of the invention according to claim 5 undergoes a phase change so as to be in close contact with the electronic component within the operating temperature range of the electronic component, and reduces the interface contact thermal resistance value to reduce the heat conduction performance. Can be increased.

本発明の相変化熱伝導性成形体によれば、熱伝導性能に優れるとともにハンドリング性及び転写性を高めることが容易である。   According to the phase change heat conductive molded body of the present invention, it is easy to improve the heat transfer performance and handleability and transferability.

以下、本発明の実施形態を詳細に説明する。
本実施形態の相変化熱伝導性成形体(以下、単に成形体という。)は、スチレン系エラストマーと、パラフィンオイルと、熱伝導性充填材と、可塑剤とを含有する相変化熱伝導性組成物(以下、単に組成物という。)から成形される。この成形体は電子部品と冷却部材との間に介在され、通電により発熱している電子部品から冷却部材への熱伝導を促進する。
Hereinafter, embodiments of the present invention will be described in detail.
The phase change heat conductive molded body of the present embodiment (hereinafter simply referred to as a molded body) is a phase change heat conductive composition containing a styrene elastomer, paraffin oil, a heat conductive filler, and a plasticizer. It is molded from a product (hereinafter simply referred to as a composition). This molded body is interposed between the electronic component and the cooling member, and promotes heat conduction from the electronic component that generates heat by energization to the cooling member.

成形体には、熱伝導性能、ハンドリング性及び転写性が具備されている。熱伝導性能は電子部品から冷却部材への熱伝導のし易さを表す指標であり、成形体の熱抵抗値や界面接触熱抵抗値に起因している。成形体の熱抵抗値は下記式により求められ、例えば成形体の熱伝導率が高いほど小さい。一方、界面接触熱抵抗値は、成形体と、電子部品及び冷却部材との界面に形成される空隙が小さいほど、即ち成形体と電子部品及び冷却部材との密着性が高いほど小さい。成形体は、これら熱抵抗値及び界面接触熱抵抗値が小さいほど電子部品から冷却部材への熱伝導を促進し、熱伝導性能に優れたものとなる。   The molded body is provided with heat conduction performance, handling properties, and transferability. The heat conduction performance is an index representing the ease of heat conduction from the electronic component to the cooling member, and is caused by the thermal resistance value and the interface contact thermal resistance value of the molded body. The thermal resistance value of the molded body is obtained by the following formula, and for example, the higher the thermal conductivity of the molded body, the smaller the thermal resistance value. On the other hand, the interfacial contact thermal resistance value is smaller as the gap formed at the interface between the molded body, the electronic component, and the cooling member is smaller, that is, as the adhesion between the molded body, the electronic component, and the cooling member is higher. As the heat resistance value and the interface contact heat resistance value are smaller, the molded body promotes heat conduction from the electronic component to the cooling member, and becomes more excellent in heat conduction performance.

熱抵抗値[℃/W]=成形体の厚み[m]/(成形体表面の面積[m2]×成形体の熱伝導率[W/(m・K)])
ハンドリング性は成形体の取扱い易さを表す指標であり、成形体の取扱い時の強度(引裂き強度等)及び硬度に起因しており、通常は常温で取扱われることから常温での強度及び硬度に起因している。一方、転写性は成形体の電子部品への取付け易さ(転写し易さ)を表す指標であり、通常は常温で転写されることから成形体の常温での硬度及び粘着性に起因している。ここで、常温とは成形体が運搬や転写に際して通常取扱われるときの温度を示し、40℃未満、例えば25℃である。
Thermal resistance value [° C./W]=molded body thickness [m] / (molded body surface area [m 2 ] × molded body thermal conductivity [W / (m · K)])
Handleability is an index that represents the ease of handling of the molded body, and is attributed to the strength (tear strength, etc.) and hardness of the molded body. Is attributed. On the other hand, transferability is an index that represents the ease of mounting a molded body to an electronic component (easy transfer), and is usually transferred at room temperature, resulting in the hardness and adhesiveness of the molded body at room temperature. Yes. Here, normal temperature refers to the temperature at which the molded body is normally handled during transportation and transfer, and is less than 40 ° C., for example, 25 ° C.

成形体は、常温での強度が高いほど運搬時の取扱いが容易であることからハンドリング性が高められ、逆に常温での強度の低下に伴って千切れ易くなることからハンドリング性が低下する。さらに、成形体は、常温での柔軟性の低下に伴って硬度が高くなり、割れ易くなってハンドリング性が低下する。逆に、成形体は常温での柔軟性の向上に伴って硬度が低下し、転写時に加えられる荷重により潰れ易くなって転写性が低下する。このため、成形体は、硬度を適宜に調整することによりハンドリング性及び転写性が高められる。加えて、成形体は、常温での粘着性が過剰に高いと電子部品への取付け(転写)が困難になって転写性が低下し、常温での粘着性が過剰に低いと電子部品から剥がれ易くなって転写性が低下する。このため、成形体は、粘着性を適宜に調整することにより転写性が高められる。この成形体は、スチレン系エラストマー等の各成分を配合及び溶融混練して組成物を調製し、その組成物を所定の形状に成形した後に冷却して固化させることにより製造される。   The higher the strength at room temperature, the easier the handling of the molded body is during handling, and the handleability is improved. Conversely, the strength is reduced as the strength at room temperature decreases, and the handling property is reduced. Further, the molded body has a higher hardness with a decrease in flexibility at room temperature, and is easily broken, resulting in a decrease in handling properties. On the other hand, the molded body has a hardness that decreases with an increase in flexibility at room temperature, and is easily crushed by a load applied during transfer, resulting in a decrease in transferability. For this reason, handling property and transferability are improved by appropriately adjusting the hardness of the molded body. In addition, if the molded product has an excessively high adhesive property at room temperature, it becomes difficult to attach (transfer) to the electronic component, resulting in a decrease in the transfer property. If the adhesive property at ordinary temperature is excessively low, the molded product peels off from the electronic component. It becomes easy and transferability falls. For this reason, as for a molded object, transferability is improved by adjusting adhesiveness suitably. This molded body is produced by blending and melting and kneading each component such as a styrene-based elastomer to prepare a composition, molding the composition into a predetermined shape, and then cooling and solidifying the composition.

スチレン系エラストマーは、パラフィンオイル等の成形体中の他の成分を成形体内に保持して成形体からブリーディング(浸み出し)することを抑制する。スチレン系エラストマーは熱可塑性を有しており、電子部品の使用温度範囲よりも高い軟化点を備えている。ここで、前記電子部品の使用温度範囲とは、電子部品が通電及び放熱されているときの温度範囲、即ち電子部品の処理能力にほとんど悪影響を及ぼさない温度範囲を指す。この使用温度範囲は電子部品の種類によって異なるが、常温よりも高く例えば40〜80℃である。   Styrenic elastomers hold other components in the molded body such as paraffin oil in the molded body and suppress bleeding (penetration) from the molded body. Styrenic elastomer has thermoplasticity and has a softening point higher than the operating temperature range of electronic components. Here, the operating temperature range of the electronic component refers to a temperature range in which the electronic component is energized and dissipated, that is, a temperature range in which the processing performance of the electronic component is hardly adversely affected. This operating temperature range varies depending on the type of electronic component, but is higher than room temperature, for example, 40 to 80 ° C.

スチレン系エラストマーの具体例としては、ポリスチレン−ポリブタジエン−ポリスチレン共重合体やポリスチレン−ポリイソプレン−ポリスチレン共重合体等のブロック共重合体が挙げられる。さらに、スチレン系エラストマーとしては、前記各ブロック共重合体の水素添加物、即ち水添スチレン系エラストマーであるスチレン−エチレン−ブチレン−スチレン共重合体(SEBS)やスチレン−エチレン−プロピレン−スチレン共重合体(SEPS)等のトリブロック共重合体が挙げられる。これらの中でも、機械的強度、耐熱性及び耐久性が優れているために水添スチレン系エラストマーが好ましく、SEBSがより好ましい。   Specific examples of the styrene elastomer include block copolymers such as polystyrene-polybutadiene-polystyrene copolymer and polystyrene-polyisoprene-polystyrene copolymer. Further, as the styrene elastomer, hydrogenated products of the respective block copolymers, that is, styrene-ethylene-butylene-styrene copolymer (SEBS) which is a hydrogenated styrene elastomer, styrene-ethylene-propylene-styrene copolymer. Triblock copolymers such as coalesced (SEPS) are exemplified. Among these, hydrogenated styrene-based elastomers are preferable due to excellent mechanical strength, heat resistance, and durability, and SEBS is more preferable.

スチレン系エラストマーの硬度Hsは70以下が好ましい。硬度Hsが70を超えると、成形体は常温での柔軟性が低下して硬度が過剰に高くなりハンドリング性が低下するおそれがある。ここで、硬度HsはJIS K 6253に従いタイプAデュロメータを用いて測定される。スチレン系エラストマーの数平均分子量の下限は60000が好ましい。数平均分子量が60000未満では、パラフィンオイル等のブリーディングが発生するおそれがある。スチレン系エラストマーの数平均分子量の上限は特に限定されないが、通常は400000程度である。   The hardness Hs of the styrene elastomer is preferably 70 or less. When the hardness Hs exceeds 70, the molded body may have low flexibility at room temperature, excessively high hardness, and handling properties may be deteriorated. Here, the hardness Hs is measured using a type A durometer according to JIS K 6253. The lower limit of the number average molecular weight of the styrene elastomer is preferably 60000. If the number average molecular weight is less than 60000, bleeding such as paraffin oil may occur. The upper limit of the number average molecular weight of the styrene elastomer is not particularly limited, but is usually about 400,000.

パラフィンオイルは常温雰囲気下において液状をなし、スチレン系エラストマーの外部可塑剤として作用する。このため、パラフィンオイルは、スチレン系エラストマーを含有する成形体を前記電子部品の使用温度範囲内で可塑化させ易くし、成形体を電子部品及び冷却部材の両方に密着させて界面接触熱抵抗値を低下させる。さらに、パラフィンオイルは柔軟性及び粘着性を有し、成形体に柔軟性及び粘着性を付与する。加えて、パラフィンオイル及び前記スチレン系エラストマーはリサイクル可能であり、成形体をリサイクル可能にしてその廃棄による環境に対する影響を低減することができる。パラフィンオイルの25℃における粘度は0.15Pa・s(150cP)以下が好ましい。粘度が0.15Pa・sを超えると組成物が高粘度となり、成形体の成形が困難になるおそれがある。   Paraffin oil is liquid in a normal temperature atmosphere and acts as an external plasticizer for the styrene elastomer. For this reason, paraffin oil makes it easy to plasticize a molded body containing a styrene elastomer within the operating temperature range of the electronic component, and the molded body is brought into close contact with both the electronic component and the cooling member so that the interface contact thermal resistance value is increased. Reduce. Furthermore, paraffin oil has a softness | flexibility and adhesiveness, and provides a softness | flexibility and adhesiveness to a molded object. In addition, the paraffin oil and the styrene-based elastomer can be recycled, and the molded product can be recycled to reduce the environmental impact of the disposal. The viscosity of the paraffin oil at 25 ° C. is preferably 0.15 Pa · s (150 cP) or less. When the viscosity exceeds 0.15 Pa · s, the composition has a high viscosity, which may make it difficult to mold the molded body.

パラフィンオイルの配合量はスチレン系エラストマー100重量部に対し300〜700重量部の割合が好ましく、400〜600重量部の割合がより好ましい。パラフィンオイルの配合量が300重量部未満では、成形体の常温での柔軟性が低くなり、硬度が過剰に高くなる。このため、成形体のハンドリング性が低下するおそれがある。さらにこのとき、成形体の常温での粘着性が過剰に低くなり、転写時に電子部品から容易に剥がれて転写性が低下するおそれがある。一方、パラフィンオイルの配合量が700重量部を超えると、成形体の常温での強度及び硬度が過剰に低くなる。このため、成形体のハンドリング性及び転写性が低下するおそれがある。さらにこのとき、成形体の常温での粘着性が過剰に高くなり、電子部品への転写が困難になって転写性が低下するおそれがある。このため、パラフィンオイルは、その配合量を前記範囲に調整することにより、成形体の常温での強度を高めるとともに硬度及び粘着性を調整してハンドリング性及び転写性を高めることができる。   The proportion of paraffin oil is preferably 300 to 700 parts by weight, more preferably 400 to 600 parts by weight, based on 100 parts by weight of the styrene elastomer. When the blending amount of the paraffin oil is less than 300 parts by weight, the flexibility of the molded body at normal temperature is lowered and the hardness is excessively increased. For this reason, there exists a possibility that the handleability of a molded object may fall. Furthermore, at this time, the adhesiveness of the molded body at room temperature becomes excessively low, and it may be easily peeled off from the electronic component at the time of transfer and the transferability may be lowered. On the other hand, when the blending amount of paraffin oil exceeds 700 parts by weight, the strength and hardness of the molded body at room temperature are excessively lowered. For this reason, there exists a possibility that the handleability and transferability of a molded object may fall. Furthermore, at this time, the adhesiveness of the molded body at room temperature becomes excessively high, which makes it difficult to transfer to an electronic component, and there is a concern that transferability may be reduced. For this reason, by adjusting the blending amount of the paraffin oil to the above range, it is possible to increase the strength of the molded body at room temperature and adjust the hardness and adhesiveness to improve the handling property and transferability.

熱伝導性充填材は、成形体の熱伝導率を高めることにより、成形体の熱伝導性能を高める。熱伝導性充填材としてはスチレン系エラストマー等の成形体中の他の成分よりも熱伝導率が高いものであれば特に限定されない。ただし、酸化アルミニウム、窒化ホウ素、窒化アルミニウム、炭化ケイ素及び二酸化ケイ素から選ばれる少なくとも一種が、熱伝導率が特に高いために好ましい。熱伝導性充填材の形状としては、球状、楕円球状、多角柱状等が挙げられる。多角柱状をなす熱伝導性充填材は、例えば熱伝導性繊維の粉砕により得られる。これらの中でも、組成物の調製時における分散性が高いとともに成形体の表面に凹凸が形成されて表面形状が悪化するのを防止するために球状又は楕円球状が好ましく、球状がより好ましい。   The thermally conductive filler increases the thermal conductivity of the molded body by increasing the thermal conductivity of the molded body. The heat conductive filler is not particularly limited as long as it has a higher thermal conductivity than other components in the molded body such as a styrene elastomer. However, at least one selected from aluminum oxide, boron nitride, aluminum nitride, silicon carbide and silicon dioxide is preferable because of its particularly high thermal conductivity. Examples of the shape of the thermally conductive filler include a spherical shape, an elliptical spherical shape, and a polygonal columnar shape. The heat conductive filler having a polygonal column shape is obtained, for example, by pulverization of heat conductive fibers. Among these, a spherical shape or an elliptical shape is preferable, and a spherical shape is more preferable in order to prevent the surface shape from being deteriorated due to high dispersibility during preparation of the composition and formation of irregularities on the surface of the molded body.

ここで、成形体の熱伝導率は、熱伝導性充填材の配合量の増加に伴って高くなる。また、組成物の粘性は、配合された熱伝導性充填材の比表面積が大きくなるに伴って高くなる。このため、熱伝導性充填材は、成形体の熱伝導率を高めるとともに組成物を低粘度にするために、大径粒子と小径粒子とが組み合わされて配合されるのが好ましい。熱伝導性充填材は、大径粒子と小径粒子とが組み合わされて配合されることにより、大径粒子間に小径粒子が配合され、大径粒子のみから構成されているときに比べて配合量を高めることができる。さらに、熱伝導性充填材は、大径粒子と小径粒子とが組み合わされて配合されることにより、小径粒子のみから構成されているときに比べて比表面積を小さくすることができる。ここで、大径粒子とはCILAS 920L(CILAS社製のレーザー回折式粒度分布測定装置)等を用いたレーザー回折散乱法により求められる平均粒径が小径粒子に比べて大きい粒子のことであり、小径粒子は同レーザー回折散乱法により求められる平均粒径が大径粒子に比べて小さい粒子のことである。   Here, the thermal conductivity of the molded body increases as the blending amount of the thermally conductive filler increases. In addition, the viscosity of the composition increases as the specific surface area of the blended thermally conductive filler increases. For this reason, it is preferable that the thermally conductive filler is blended in combination of large diameter particles and small diameter particles in order to increase the thermal conductivity of the molded body and to make the composition have a low viscosity. Compared to the case where the heat conductive filler is composed of a combination of large particles and small particles, the small particles are mixed between the large particles, and the amount of the heat conductive filler is composed only of the large particles. Can be increased. Furthermore, the heat conductive filler can be reduced in specific surface area compared to the case where the heat conductive filler is composed of only small-diameter particles by blending large-diameter particles and small-diameter particles. Here, the large-diameter particles are particles whose average particle diameter obtained by a laser diffraction scattering method using CILAS 920L (laser diffraction type particle size distribution measuring device manufactured by CILAS) or the like is larger than that of small-diameter particles, Small-diameter particles are particles whose average particle diameter determined by the laser diffraction scattering method is smaller than that of large-diameter particles.

大径粒子の形状は、球状又は楕円球状が成形体の表面形状の悪化を防止することができるために好ましい。大径粒子のレーザー回折散乱法により求められる平均粒径は10〜20μmが好ましい。大径粒子の平均粒径が10μm未満では、熱伝導性充填材の配合量が過剰に高くなり、熱伝導性充填材の比表面積が大きくなって組成物が高粘度になるおそれがある。一方、20μmを超えると、成形体の表面形状が悪化するおそれがある。小径粒子のレーザー回折散乱法により求められる平均粒径は1〜5μmが好ましい。小径粒子の平均粒径が1μm未満では、大径粒子間に小径粒子が過剰に配合され、熱伝導性充填材の配合量が高く組成物が高粘度になるおそれがある。一方、5μmを超えると、大径粒子間に小径粒子が十分配合されず、熱伝導性充填材の配合量が低下するおそれがある。   As the shape of the large-diameter particles, a spherical shape or an elliptical shape is preferable because the deterioration of the surface shape of the molded body can be prevented. The average particle size determined by the laser diffraction scattering method for large particles is preferably 10 to 20 μm. When the average particle size of the large-diameter particles is less than 10 μm, the blending amount of the heat conductive filler is excessively high, and the specific surface area of the heat conductive filler is increased, and the composition may have a high viscosity. On the other hand, if it exceeds 20 μm, the surface shape of the molded article may be deteriorated. The average particle size determined by the laser diffraction scattering method for small-diameter particles is preferably 1 to 5 μm. When the average particle size of the small-diameter particles is less than 1 μm, the small-diameter particles are excessively blended between the large-diameter particles, and the blending amount of the heat conductive filler may be high and the composition may have a high viscosity. On the other hand, when it exceeds 5 μm, the small-diameter particles are not sufficiently blended between the large-diameter particles, and the blending amount of the heat conductive filler may be reduced.

熱伝導性充填材の配合量は、スチレン系エラストマー100重量部に対し1000〜6000重量部の割合が好ましく、2500〜5000重量部の割合がより好ましい。熱伝導性充填材は、1000重量部以上配合されることにより成形体の熱伝導率を1.5W/(m・K)以上にまで高めることができる。しかし、熱伝導性充填材の配合量が6000重量部を超えると、組成物が高粘度となるおそれがある。このため、熱伝導性充填材は、その配合量を前記範囲にすることにより、成形体の熱伝導率を高めるとともに組成物を低粘度にすることができる。ここで、熱伝導性充填材が大径粒子と小径粒子とを組み合わされて配合されるときは、前記配合量は大径粒子及び小径粒子の各配合量の合計を示す。   The blending amount of the heat conductive filler is preferably 1000 to 6000 parts by weight, more preferably 2500 to 5000 parts by weight with respect to 100 parts by weight of the styrene elastomer. When the heat conductive filler is blended in an amount of 1000 parts by weight or more, the thermal conductivity of the molded body can be increased to 1.5 W / (m · K) or more. However, when the blending amount of the heat conductive filler exceeds 6000 parts by weight, the composition may have a high viscosity. For this reason, a heat conductive filler can make a composition low viscosity while raising the heat conductivity of a molded object by making the compounding quantity into the said range. Here, when the thermally conductive filler is blended by combining large-diameter particles and small-diameter particles, the blending amount indicates the total blending amount of the large-diameter particles and the small-diameter particles.

可塑剤の凝固点は常温よりも高い40〜60℃の範囲内である。このため、可塑剤は常温雰囲気下において固体状をなし、成形体の常温での強度及び硬度を高める。さらに、可塑剤は、常温よりも高い温度の雰囲気下において液状をなし、パラフィンオイルと同様にスチレン系エラストマーの外部可塑剤として作用する。このため、液状をなす可塑剤は、パラフィンオイルとともに成形体を前記電子部品の使用温度範囲内で可塑化させ易くして界面接触熱抵抗値を低下させる。加えて、可塑剤は柔軟性を有し、かつパラフィンオイルに比べて低い粘着性を有しており、成形体に柔軟性及び粘着性を付与する。可塑剤の凝固点が40℃未満の場合、その可塑剤は常温雰囲気下において液状をなす。このため、成形体は常温雰囲気下で可塑化し、柔軟性が高められて硬度が過剰に低下する。よって、成形体の転写性は低下する。一方、可塑剤の凝固点が60℃を超えると、その可塑剤は前記電子部品の使用温度範囲内の低温側で固体状をなす。このため、成形体は、電子部品の使用温度範囲内の低温側雰囲気下では可塑化せず、界面接触熱抵抗値を低下させることができない。よって、成形体は熱伝導性能を高めることができない。   The freezing point of the plasticizer is in the range of 40-60 ° C., which is higher than normal temperature. For this reason, the plasticizer is solid in a normal temperature atmosphere, and increases the strength and hardness of the molded body at normal temperature. Furthermore, the plasticizer is in a liquid state in an atmosphere at a temperature higher than normal temperature, and acts as an external plasticizer for the styrenic elastomer, like paraffin oil. For this reason, the liquid plasticizer makes it easy to plasticize the molded body within the operating temperature range of the electronic component together with the paraffin oil to reduce the interface contact thermal resistance value. In addition, the plasticizer has flexibility and has low adhesiveness compared to paraffin oil, and imparts flexibility and adhesiveness to the molded body. When the freezing point of the plasticizer is less than 40 ° C., the plasticizer becomes liquid in a normal temperature atmosphere. For this reason, a molded object is plasticized in normal temperature atmosphere, a softness | flexibility is improved and hardness falls excessively. Therefore, the transferability of the molded body is lowered. On the other hand, when the freezing point of the plasticizer exceeds 60 ° C., the plasticizer becomes solid on the low temperature side within the use temperature range of the electronic component. For this reason, a molded object does not plasticize in the low temperature side atmosphere within the use temperature range of an electronic component, and cannot reduce an interface contact thermal resistance value. Therefore, a molded object cannot improve heat conduction performance.

可塑剤の具体例としては、ステアリン酸(凝固点:58〜60℃)、フェノールホルムアルデヒド樹脂、トリフェニルホスフェート(リン酸エステル、凝固点:48〜50℃)等が挙げられる。これらは単独で使用されてもよいし、二種以上が組み合わされて使用されてもよい。これらの中でも、トリフェニルホスフェートが好ましい。このトリフェニルホスフェートは、スチレン系エラストマーに対する非相溶性を有するとともに非粘着性を有し、凝固点よりも高い温度のときには溶解して水のように非常に低粘度の液体となる。このため、トリフェニルホスフェートは、常温雰囲気下における成形体の強度及び硬度を高め、かつ前記電子部品の使用温度範囲内の雰囲気下において成形体を可塑化させ易くする。さらに、トリフェニルホスフェートは、成形体の常温での粘着性を低下させて転写性を高め、しかも不燃性を有するために成形体に難燃性を付与することができる。   Specific examples of the plasticizer include stearic acid (freezing point: 58 to 60 ° C.), phenol formaldehyde resin, triphenyl phosphate (phosphate ester, freezing point: 48 to 50 ° C.), and the like. These may be used alone or in combination of two or more. Among these, triphenyl phosphate is preferable. This triphenyl phosphate has incompatibility with the styrenic elastomer and is non-adhesive, and dissolves at a temperature higher than the freezing point to form a very low viscosity liquid such as water. For this reason, triphenyl phosphate increases the strength and hardness of the molded body in a normal temperature atmosphere, and facilitates plasticizing the molded body in an atmosphere within the operating temperature range of the electronic component. Furthermore, triphenyl phosphate reduces the adhesiveness of the molded body at room temperature to improve transferability, and has nonflammability, and therefore can impart flame retardancy to the molded body.

可塑剤の配合量はスチレン系エラストマー100重量部に対し50〜400重量部の割合が好ましい。可塑剤の配合量が50重量部未満では、成形体の常温での強度が過剰に低くなる。このため、成形体のハンドリング性が低下するおそれがある。さらにこのとき、成形体の常温での硬度が過剰に低くなるとともに常温での粘着性が過剰に高くなる。このため、成形体の転写性が低下するおそれがある。一方、可塑剤の配合量が400重量部を超えると、成形体の常温での硬度が過剰に高くなる。このため、成形体のハンドリング性が低下するおそれがある。さらにこのとき、成形体の常温での粘着性が過剰に低くなる。このため、成形体の転写性が低下するおそれがある。よって、可塑剤の配合量を前記範囲に調整することにより、成形体の常温での強度を高めてハンドリング性を高めるとともに硬度及び粘着性を調整してハンドリング性及び転写性を高めることができる。組成物中には、前記各成分以外のその他の成分として粘着剤、補強剤、着色剤、耐熱向上剤等を配合することも可能である。   The blending amount of the plasticizer is preferably 50 to 400 parts by weight with respect to 100 parts by weight of the styrene elastomer. When the blending amount of the plasticizer is less than 50 parts by weight, the strength of the molded body at room temperature becomes excessively low. For this reason, there exists a possibility that the handleability of a molded object may fall. Furthermore, at this time, the hardness of the molded body at room temperature is excessively lowered and the adhesiveness at room temperature is excessively increased. For this reason, there exists a possibility that the transferability of a molded object may fall. On the other hand, when the compounding amount of the plasticizer exceeds 400 parts by weight, the hardness of the molded body at room temperature becomes excessively high. For this reason, there exists a possibility that the handleability of a molded object may fall. Further, at this time, the adhesiveness of the molded body at room temperature is excessively lowered. For this reason, there exists a possibility that the transferability of a molded object may fall. Therefore, by adjusting the blending amount of the plasticizer within the above range, it is possible to improve the handling property and transferability by increasing the strength of the molded body at room temperature to improve the handling property and adjusting the hardness and the adhesiveness. In the composition, an adhesive, a reinforcing agent, a colorant, a heat resistance improver, and the like can be blended as other components other than the above-described components.

成形体は、前記電子部品の使用温度範囲よりも高い温度で軟化するスチレン系エラストマー、スチレン系エラストマーの外部可塑剤として作用するパラフィンオイル及び凝固点が40〜60℃の範囲内である可塑剤を含有している。それにより、可塑化温度(相変化温度)がスチレン系エラストマーの軟化点よりも低く、前記電子部品の使用温度範囲と一致している。成形体の形状としてはブロック状、シート状等が挙げられ、発熱電子部品から冷却部材への熱伝導の促進効果が高いためにシート状が好ましい。シート状をなす成形体、即ち熱伝導性シートは、前記式に示すように、厚みを薄くすることにより熱抵抗値を低下させ熱伝導性能を高めることができる。   The molded body contains a styrene elastomer that softens at a temperature higher than the operating temperature range of the electronic component, paraffin oil that acts as an external plasticizer for the styrene elastomer, and a plasticizer that has a freezing point in the range of 40 to 60 ° C. doing. Thereby, the plasticization temperature (phase change temperature) is lower than the softening point of the styrene-based elastomer, and is consistent with the operating temperature range of the electronic component. Examples of the shape of the molded body include a block shape and a sheet shape, and the sheet shape is preferable because the effect of promoting heat conduction from the heat generating electronic component to the cooling member is high. As shown in the above formula, the sheet-like molded body, that is, the heat conductive sheet, can have a reduced thermal resistance value and improved heat conduction performance by reducing the thickness.

このため、前記電子部品の使用温度範囲未満の雰囲気下における熱伝導性シートの厚み、即ち40℃未満のときの熱伝導性シートの厚みは50〜300μmが好ましい。40℃未満のときの熱伝導性シートの厚みが50μm未満では、熱伝導性シートの常温での強度が低下するおそれがある。一方、厚みが300μmを超えると、熱伝導性シートが厚くなり熱抵抗値が高くなるおそれがある。さらに、前記電子部品の使用温度範囲以上の温度の雰囲気下における熱伝導性シートの厚み、即ち40℃以上のときの熱伝導性シートの厚みは100μm以下が好ましい。40℃以上のときの厚みが100μmを超えると、熱伝導性シートの熱抵抗値が高くなるおそれがある。   For this reason, the thickness of the heat conductive sheet in an atmosphere below the operating temperature range of the electronic component, that is, the thickness of the heat conductive sheet when the temperature is less than 40 ° C. is preferably 50 to 300 μm. If the thickness of the heat conductive sheet at less than 40 ° C. is less than 50 μm, the strength of the heat conductive sheet at normal temperature may be reduced. On the other hand, if the thickness exceeds 300 μm, the thermal conductive sheet may be thick and the thermal resistance value may be increased. Furthermore, the thickness of the heat conductive sheet in an atmosphere having a temperature equal to or higher than the operating temperature range of the electronic component, that is, the thickness of the heat conductive sheet at 40 ° C. or higher is preferably 100 μm or less. When the thickness at 40 ° C. or higher exceeds 100 μm, the thermal resistance value of the thermal conductive sheet may be increased.

成形体を製造するときには、まずスチレン系エラストマーに可塑剤等の各成分を配合し、ヘンシェルミキサー等の密閉型混合機を用いて各成分が均一に分散するまで溶融混練して組成物を調製する。次いで、組成物をバーコータ法、ドクターブレード法、押出成形法(Tダイ法)、カレンダー成形法、プレス成形法等によって所定の形状に成形した後、冷却して固化させることにより成形体を得る。続いて、成形体として例えば熱伝導性シートが得られたときには、熱伝導性シートの両面に離型フィルムを貼着する。離型フィルムはポリエチレンテレフタレート(PET)等の合成樹脂材料により形成され、熱伝導性シートを保護する。   When producing a molded body, first, each component such as a plasticizer is blended into a styrene elastomer, and a composition is prepared by melt-kneading until each component is uniformly dispersed using a closed mixer such as a Henschel mixer. . Next, the composition is molded into a predetermined shape by a bar coater method, a doctor blade method, an extrusion molding method (T-die method), a calendar molding method, a press molding method, or the like, and then cooled and solidified to obtain a molded body. Subsequently, when, for example, a heat conductive sheet is obtained as a molded body, release films are attached to both surfaces of the heat conductive sheet. The release film is formed of a synthetic resin material such as polyethylene terephthalate (PET) and protects the heat conductive sheet.

両面に離型フィルムが貼着された熱伝導性シートを電子部品に取付ける(転写する)ときには、前記電子部品の使用温度範囲よりも低い常温雰囲気下で一方の離型フィルムを熱伝導性シートから剥離した後、露出した熱伝導性シートの表面を電子部品に貼付ける。このとき、熱伝導性シートが電子部品に密着するように、その熱伝導性シートに196〜392kPa(2〜4kgf/cm2)の荷重を加え、熱伝導性シートを電子部品に固定する。続いて、他方の離型フィルムを熱伝導性シートから剥離した後、露出した熱伝導性シートの表面に冷却部材を載置する。このとき、冷却部材が熱伝導性シートに密着するように、冷却部材に196〜392kPaの荷重を加え、熱伝導性シートを冷却部材にも固定する。 When attaching (transferring) a heat conductive sheet having a release film attached to both sides to an electronic component, one release film is removed from the heat conductive sheet in a room temperature atmosphere lower than the operating temperature range of the electronic component. After peeling, the exposed surface of the heat conductive sheet is attached to the electronic component. At this time, a load of 196 to 392 kPa ( 2 to 4 kgf / cm 2 ) is applied to the thermally conductive sheet so that the thermally conductive sheet is in close contact with the electronic component, and the thermally conductive sheet is fixed to the electronic component. Subsequently, after peeling off the other release film from the heat conductive sheet, a cooling member is placed on the exposed surface of the heat conductive sheet. At this time, a load of 196 to 392 kPa is applied to the cooling member so that the cooling member is in close contact with the heat conductive sheet, and the heat conductive sheet is also fixed to the cooling member.

さて、電子部品に転写された熱伝導性シートは、電子部品の通電による発熱に伴って加熱される。そして、熱伝導性シートは、電子部品の温度がその使用温度範囲内にまで上昇したときは、相変化温度にまで加熱されて可塑化を引き起こされる。このため、熱伝導性シートは、電子部品及び冷却部材の表面形状に追従して電子部品及び冷却部材に密着する。よって、熱伝導性シートは電子部品及び冷却部材との界面接触熱抵抗値が低下し、電子部品から冷却部材への熱伝導を促進して放熱する。さらに、熱伝導性シートの可塑化に伴ってその厚さが薄くなり、熱抵抗値が低下して熱伝導がより一層促進する。   Now, the heat conductive sheet transcribe | transferred to the electronic component is heated with the heat_generation | fever by electricity supply of an electronic component. And when the temperature of an electronic component rises in the use temperature range, a heat conductive sheet is heated even to a phase change temperature, and plasticization is caused. For this reason, a heat conductive sheet follows the surface shape of an electronic component and a cooling member, and closely_contact | adheres to an electronic component and a cooling member. Therefore, the thermal conductive sheet has a lower interface contact thermal resistance value between the electronic component and the cooling member, and promotes heat conduction from the electronic component to the cooling member to dissipate heat. Further, as the heat conductive sheet is plasticized, its thickness is reduced, the heat resistance value is lowered, and heat conduction is further promoted.

前記の実施形態によって発揮される効果について、以下に記載する。
・ 本実施形態の成形体はスチレン系エラストマー、パラフィンオイル及び可塑剤を含有する組成物により成形されている。可塑剤は40〜60℃の範囲内の凝固点を有し、常温雰囲気下において固体状をなし、成形体の強度及び硬度を高める。このため、成形体は、その運搬等の取扱いに際して千切れ難いとともに潰れ難い。
The effects exhibited by the above embodiment will be described below.
-The molded object of this embodiment is shape | molded by the composition containing a styrene-type elastomer, paraffin oil, and a plasticizer. The plasticizer has a freezing point in the range of 40 to 60 ° C., forms a solid in a normal temperature atmosphere, and increases the strength and hardness of the molded body. For this reason, a molded object is hard to tear at the time of handling, such as the conveyance, and is hard to be crushed.

さらに、可塑剤は、常温よりも高い温度の雰囲気下において液状をなし、パラフィンオイルとともに成形体を前記電子部品の使用温度範囲内で可塑化させ易くする。このため、パラフィンオイルの含有量を低減させることができる。よって、パラフィンオイルの増量に起因する常温での強度及び硬度の低下や粘着性の増加を未然に防止でき、電子部品への転写が容易な成形体が得られる。   Furthermore, the plasticizer is in a liquid state in an atmosphere at a temperature higher than normal temperature, and facilitates plasticizing the molded body together with the paraffin oil within the operating temperature range of the electronic component. For this reason, content of paraffin oil can be reduced. Therefore, a decrease in strength and hardness at room temperature and an increase in adhesiveness due to an increase in the amount of paraffin oil can be prevented, and a molded body that can be easily transferred to an electronic component can be obtained.

・ 成形体は熱伝導性充填材を含有し、その相変化温度が前記電子部品の使用温度範囲と一致している。このため、成形体の熱伝導率が高められ、電子部品が発熱してその温度が40〜80℃の温度範囲内にまで上昇したときには、成形体の可塑化が引き起こされて電子部品及び冷却部材に密着する。よって、成形体は優れた熱伝導性能を発揮することができる。   -A molded object contains a heat conductive filler and the phase change temperature corresponds with the use temperature range of the said electronic component. Therefore, when the thermal conductivity of the molded body is increased and the electronic component generates heat and its temperature rises to a temperature range of 40 to 80 ° C., the molded body is plasticized, and the electronic component and the cooling member Close contact with. Therefore, a molded object can exhibit the outstanding heat conductive performance.

・ 熱伝導性充填材は、大径粒子と小径粒子とが組み合わされて配合されるのが好ましい。この場合には、成形体の熱伝導率が高まり、かつ組成物を低粘度にして成形体を容易に製造することができる。このとき、小径粒子の大径粒子間への配合量を高めるために、小径粒子の平均粒径は大径粒子の平均粒径の7分の1程度が好ましい。   The heat conductive filler is preferably blended with a combination of large diameter particles and small diameter particles. In this case, the thermal conductivity of the molded body is increased, and the molded body can be easily produced with a low viscosity composition. At this time, in order to increase the blending amount of the small-diameter particles between the large-diameter particles, the average particle diameter of the small-diameter particles is preferably about 1/7 of the average particle diameter of the large-diameter particles.

尚、本実施形態は、次のように変更して具体化することも可能である。
・ 前記成形体の表面や内部にフィルム、シート、不織布、織布等を貼着又は埋没させてもよい。この場合には、運搬や転写時等での成形体の作業性を向上させたり成形体を補強したりすることができる。
In addition, this embodiment can also be changed and embodied as follows.
-A film, a sheet, a nonwoven fabric, a woven fabric, or the like may be attached or buried on the surface or inside of the molded body. In this case, it is possible to improve the workability of the molded body during transportation or transfer, or to reinforce the molded body.

次に、試験例及び比較例を挙げて前記実施形態をさらに具体的に説明する。
(試験例1〜5及び比較例1)
試験例1においては、スチレン系エラストマーにパラフィンオイルを混合し、さらに可塑剤としてのトリフェニルホスフェート及び熱伝導性充填材としての球状酸化アルミニウム(球状アルミナ)を混合した。ここで、球状アルミナは、大径粒子の球状アルミナ(昭和電工株式会社製のAS−20、平均粒径:20μm)と小径粒子の球状アルミナ(昭和電工株式会社製のA−SAMPLE、平均粒径:3μm)とをそれぞれ5:2(質量比)の割合で混合したものを用いた。次いで、前記各成分の混合物を溶融混練して組成物を調製した。そして、その組成物から、加熱延伸機によって成形体としての熱伝導性シート(厚さ:0.1mm)を得た。組成物の調製時における各成分の配合量(重量部)及び得られた成形体中における各成分の含有量(重量%)をそれぞれ表1に示す。
Next, the embodiment will be described more specifically with reference to test examples and comparative examples.
(Test Examples 1 to 5 and Comparative Example 1)
In Test Example 1, paraffin oil was mixed with a styrene elastomer, and further, triphenyl phosphate as a plasticizer and spherical aluminum oxide (spherical alumina) as a heat conductive filler were mixed. Here, spherical alumina is composed of large-diameter spherical alumina (AS-20 manufactured by Showa Denko KK, average particle size: 20 μm) and small-diameter spherical alumina (A-SAMPLE manufactured by Showa Denko KK, average particle size). : 3 μm) in a ratio of 5: 2 (mass ratio). Subsequently, the mixture of each said component was melt-kneaded and the composition was prepared. And the heat conductive sheet (thickness: 0.1 mm) as a molded object was obtained from the composition with the heating drawing machine. Table 1 shows the blending amount (parts by weight) of each component at the time of preparing the composition and the content (% by weight) of each component in the obtained molded article.

試験例2〜5及び比較例1においては、組成物の調製時における各成分の配合量を表1に示すように変更した以外は、試験例1と同様にして熱伝導性シートを得た。そして、各例の熱伝導性シートについて、下記の各項目に関し評価及び測定を行った。その結果を表1に示す。   In Test Examples 2 to 5 and Comparative Example 1, a heat conductive sheet was obtained in the same manner as in Test Example 1 except that the amount of each component at the time of preparing the composition was changed as shown in Table 1. And about the heat conductive sheet of each example, evaluation and measurement were performed regarding the following items. The results are shown in Table 1.

<熱抵抗値>
各例の熱伝導性シートを、発熱量75Wの電子部品と冷却部材としての冷却フィンとの間に介在させた状態で、加圧機により39.2N(4kgf)の荷重を5分間加えることによって、電子部品と冷却フィンとの間に貼着した。次いで、5分経過後の電子部品と冷却フィンとの温度差を算出し、該温度差から熱抵抗値を求めた。
<Thermal resistance value>
By applying a load of 39.2 N (4 kgf) for 5 minutes by a pressurizing machine with the heat conductive sheet of each example interposed between an electronic component having a calorific value of 75 W and a cooling fin as a cooling member, It stuck between the electronic component and the cooling fin. Next, a temperature difference between the electronic component and the cooling fin after 5 minutes was calculated, and a thermal resistance value was obtained from the temperature difference.

<シート強度>
各例の熱伝導性シートの両面にPET製の離型フィルムをそれぞれ貼着した。ここで、熱伝導性シートと離型フィルムとの貼着は、加圧機により39.2Nの荷重を5分間加えることにより行った。次に、一方の離型フィルムを熱伝導性シートから剥離した。そして、離型フィルム剥離後の熱伝導性シートを目視により観察し、熱伝導性シートのシート強度について評価した。尚、全ての試験は25℃で行った。
<Sheet strength>
A release film made of PET was adhered to both sides of the heat conductive sheet of each example. Here, sticking of a heat conductive sheet and a release film was performed by applying the load of 39.2N for 5 minutes with a pressurizer. Next, one release film was peeled from the heat conductive sheet. And the heat conductive sheet after peeling release film was observed visually, and the sheet strength of the heat conductive sheet was evaluated. All tests were performed at 25 ° C.

ここで、表1において、「優良」とは、熱伝導性シートに千切れやひび割れが発生していないことを示し、「良」とは熱伝導性シートにひび割れが若干発生しているが実用上問題ないことを示す。また、「千切れ易い」とは、熱伝導性シートに千切れが発生しており離型フィルムの剥離に伴い熱伝導性シートが千切れ易く実用上問題があることを示す。   Here, in Table 1, “excellent” indicates that the thermal conductive sheet is not broken or cracked, and “good” indicates that the thermal conductive sheet is slightly cracked but is practically used. Indicates that there is no problem. Further, “easy to break” means that the thermal conductive sheet is broken into pieces, and the thermal conductive sheet is easily cut off as the release film is peeled off.

<シート硬度>
硬度計(TYPE−A又はTYPE−E、JIS K 6253準拠)を用いて各例の熱伝導性シートのシート硬度を測定した。
<Sheet hardness>
The sheet hardness of the heat conductive sheet of each example was measured using a hardness meter (TYPE-A or TYPE-E, JIS K 6253 compliant).

<転写時の硬度及び粘着性>
前記<シート強度>の測定時と同様にして各例の熱伝導性シートの両面に離型フィルムを貼着した後、一方の離型フィルムを熱伝導性シートから剥離した。そして、熱伝導性シートの露出した表面を加圧機により荷重39.2Nで電子部品表面に押し付けた後、熱伝導性シートから加圧機を離間させて熱伝導性シートに加えられていた荷重を取除いた。そして、熱伝導性シートの転写時の硬度及び粘着性について目視により評価した。尚、全ての試験は25℃で行った。
<Hardness and adhesiveness during transfer>
In the same manner as in the measurement of <Sheet Strength>, a release film was attached to both surfaces of the heat conductive sheet of each example, and then one release film was peeled from the heat conductive sheet. Then, after the exposed surface of the heat conductive sheet is pressed against the surface of the electronic component with a load of 39.2 N by a pressurizer, the load applied to the heat conductive sheet is removed by separating the pressurizer from the heat conductive sheet. Excluded. And the hardness and adhesiveness at the time of transfer of a heat conductive sheet were evaluated visually. All tests were performed at 25 ° C.

ここで、表1中の転写時の硬度について「潰れない」とは荷重による熱伝導性シートの潰れを目視により確認することができなかったことを示し、「潰れる」とは荷重によって熱伝導性シートが潰れていたことを目視により確認したことを示す。一方、粘着性について「優良」とは、熱伝導性シートが転写に適した粘着性を有し、加圧機から容易に剥がれて電子部品に接着したことを示す。「良」とは、熱伝導性シートが「優良」に比べて若干低い粘着性を有しているが、加圧機から剥がれて電子部品に接着し実用上問題ないことを示す。また、「べたつく」とは熱伝導性シートが過剰な粘着性を有して加圧機に接着し、電子部品への転写が困難であり実用上問題があることを示す。   Here, with respect to the hardness at the time of transfer in Table 1, “not crushed” means that the heat conductive sheet was not crushed by the load, and “crushed” means the heat conductivity by the load. It shows having confirmed visually that the sheet | seat was crushed. On the other hand, “excellent” in terms of tackiness indicates that the heat conductive sheet has tackiness suitable for transfer and easily peeled off from the pressurizer and adhered to the electronic component. “Good” indicates that the heat conductive sheet has a slightly lower adhesiveness than “excellent”, but peels off from the pressurizer and adheres to the electronic component, and there is no practical problem. Further, “stickiness” means that the heat conductive sheet has excessive adhesiveness and adheres to a pressurizing machine, which makes it difficult to transfer to an electronic component and has a practical problem.

<転写性>
前記<硬度及び粘着性>の結果から、熱伝導性シートの転写性について評価した。ここで、表1中の転写性について「優良」とは、熱伝導性シートの常温での硬度及び粘着性が転写に非常に適しており、熱伝導性シートを電子部品に容易に転写することができたことを示す。さらに、「良」とは、熱伝導性シートの常温での硬度及び粘着性が「優良」に比べて劣るものの実用上の転写において問題なく、熱伝導性シートを電子部品に転写できたことを示す。また、「転写できず」とは、熱伝導性シートの硬度及び粘着性が転写に適しておらず、熱伝導性シートが潰れたり加圧機に接着して電子部品に転写できなかったことを示す。
<Transferability>
From the results of <Hardness and Adhesiveness>, the transferability of the heat conductive sheet was evaluated. Here, “excellent” for the transferability in Table 1 means that the thermal conductivity of the thermal conductive sheet at room temperature is very suitable for transfer, and the thermal conductive sheet is easily transferred to an electronic component. It shows that it was possible. Furthermore, “good” means that the heat conductive sheet could be transferred to an electronic component without any problem in practical transfer, although the hardness and adhesiveness at room temperature of the heat conductive sheet were inferior to “excellent”. Show. “Unable to transfer” means that the hardness and adhesiveness of the heat conductive sheet are not suitable for transfer, and the heat conductive sheet was crushed or adhered to a pressure machine and could not be transferred to an electronic component. .

Figure 2005281346
El:スチレン系エラストマー(旭化成株式会社製のタフテックH1052)
PO:パラフィンオイル(出光興産株式会社製のPW−90)
Al:球状アルミナ
TPP:トリフェニルホスフェート(大八化学工業株式会社製)
表1に示すように、試験例1〜5においては各項目について優れた評価が得られた。このため、各試験例の熱伝導性シートは優れた熱伝導性能を有し、さらにハンドリング性及び転写性を高めることができた。ちなみに、各試験例の熱伝導性シートは40〜80℃内でそれぞれ可塑化したことが確認された。
Figure 2005281346
El: Styrene elastomer (Tuftec H1052 manufactured by Asahi Kasei Corporation)
PO: Paraffin oil (PW-90 manufactured by Idemitsu Kosan Co., Ltd.)
Al: spherical alumina TPP: triphenyl phosphate (manufactured by Daihachi Chemical Industry Co., Ltd.)
As shown in Table 1, excellent evaluation was obtained for each item in Test Examples 1 to 5. For this reason, the heat conductive sheet of each test example had excellent heat conduction performance, and was able to further improve handling and transferability. Incidentally, it was confirmed that the heat conductive sheet of each test example was plasticized within 40 to 80 ° C.

さらに、表1に示すように、熱伝導性シートは、トリフェニルホスフェートのスチレン系エラストマーに対する割合(TPP/El)を0.5〜3.9に設定することにより、シート強度、硬度及び粘着性に非常に優れハンドリング性及び転写性をより高めることができた。ここで、TPP/Elは、熱伝導性シートにおけるトリフェニルホスフェートの含有量をスチレン系エラストマーの含有量で除算することにより求められる。   Furthermore, as shown in Table 1, the heat conductive sheet has a sheet strength, hardness and adhesiveness by setting the ratio of triphenyl phosphate to styrene elastomer (TPP / El) to 0.5 to 3.9. It was extremely excellent in handling property and transferability. Here, TPP / El is calculated | required by dividing the content of the triphenyl phosphate in a heat conductive sheet by content of a styrene-type elastomer.

さらに、前記実施形態より把握できる技術的思想について以下に記載する。
・ 前記可塑剤の含有量をスチレン系エラストマーの含有量で除算することにより求められる可塑剤のスチレン系エラストマーに対する割合が0.5〜3.9である請求項1から請求項5のいずれか一項に記載の相変化熱伝導性成形体。この構成によれば、ハンドリング性及び転写性を高めることができる。
Further, the technical idea that can be grasped from the embodiment will be described below.
The ratio of the plasticizer to the styrenic elastomer obtained by dividing the plasticizer content by the styrenic elastomer content is 0.5 to 3.9. The phase change thermally conductive molded article according to Item. According to this configuration, handling and transferability can be improved.

Claims (5)

スチレン系エラストマーと、パラフィンオイルと、熱伝導性充填材と、凝固点が40〜60℃の範囲内である可塑剤とを含有する相変化熱伝導性組成物により成形されていることを特徴とする相変化熱伝導性成形体。 It is formed by a phase change heat conductive composition containing a styrene elastomer, paraffin oil, a heat conductive filler, and a plasticizer having a freezing point in the range of 40 to 60 ° C. Phase change heat conductive molding. スチレン系エラストマーと、パラフィンオイルと、熱伝導性充填材と、トリフェニルホスフェートからなる可塑剤とを含有する相変化熱伝導性組成物により成形されていることを特徴とする相変化熱伝導性成形体。 Phase change heat conductive molding characterized by being molded from a phase change heat conductive composition containing a styrenic elastomer, paraffin oil, a heat conductive filler, and a plasticizer comprising triphenyl phosphate. body. 前記可塑剤は、スチレン系エラストマー100重量部に対し50〜400重量部の割合で含有されている請求項1又は請求項2に記載の相変化熱伝導性成形体。 The phase change heat conductive molded body according to claim 1 or 2, wherein the plasticizer is contained at a ratio of 50 to 400 parts by weight with respect to 100 parts by weight of the styrene elastomer. シート状をなし、40℃未満のときの厚みが50〜300μmに設定されている請求項1から請求項3のいずれか一項に記載の相変化熱伝導性成形体。 The phase change heat conductive molded body according to any one of claims 1 to 3, wherein the phase change is formed in a sheet shape and has a thickness of less than 40 ° C set to 50 to 300 µm. 40〜80℃の温度範囲内で相変化を引き起こす請求項1から請求項4のいずれか一項に記載の相変化熱伝導性成形体。 The phase change heat conductive molded body according to any one of claims 1 to 4, which causes a phase change within a temperature range of 40 to 80 ° C.
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JP2018047660A (en) * 2016-09-23 2018-03-29 日本ゼオン株式会社 Transfer method and transfer device for heat conductive sheet
JP2020122987A (en) * 2016-09-23 2020-08-13 日本ゼオン株式会社 Transfer method and transfer device of heat conduction sheet
JP2021059671A (en) * 2019-10-08 2021-04-15 アイシン化工株式会社 Composition for heat-radiation molding

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JP2001310984A (en) * 2000-04-28 2001-11-06 Efuko Kk Thermal conductive moldings
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JP2016210957A (en) * 2015-05-13 2016-12-15 アイシン化工株式会社 Heat storage polymer molded body
JP2018047660A (en) * 2016-09-23 2018-03-29 日本ゼオン株式会社 Transfer method and transfer device for heat conductive sheet
JP2020122987A (en) * 2016-09-23 2020-08-13 日本ゼオン株式会社 Transfer method and transfer device of heat conduction sheet
JP2021059671A (en) * 2019-10-08 2021-04-15 アイシン化工株式会社 Composition for heat-radiation molding
JP7211923B2 (en) 2019-10-08 2023-01-24 アイシン化工株式会社 Composition for heat-dissipating moldings

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