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JPH0322916B2 - - Google Patents
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JPH0322916B2 - - Google Patents

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Publication number
JPH0322916B2
JPH0322916B2 JP13121682A JP13121682A JPH0322916B2 JP H0322916 B2 JPH0322916 B2 JP H0322916B2 JP 13121682 A JP13121682 A JP 13121682A JP 13121682 A JP13121682 A JP 13121682A JP H0322916 B2 JPH0322916 B2 JP H0322916B2
Authority
JP
Japan
Prior art keywords
thermal conductivity
heat
mhr
electrical insulation
resin
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired
Application number
JP13121682A
Other languages
Japanese (ja)
Other versions
JPS5922974A (en
Inventor
Katsutoshi Yoneya
Hiroshi Inoe
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Toshiba Corp
Original Assignee
Tokyo Shibaura Electric Co Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Tokyo Shibaura Electric Co Ltd filed Critical Tokyo Shibaura Electric Co Ltd
Priority to JP13121682A priority Critical patent/JPS5922974A/en
Publication of JPS5922974A publication Critical patent/JPS5922974A/en
Publication of JPH0322916B2 publication Critical patent/JPH0322916B2/ja
Granted legal-status Critical Current

Links

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  • Adhesives Or Adhesive Processes (AREA)

Description

【発明の詳細な説明】[Detailed description of the invention]

[発明の技術分野] この発明は熱伝導性、電気絶縁性および耐熱性
のすぐれた熱硬化型耐熱性接着剤に関する。 [発明の技術的背景およびその問題点] 従来から加熱したり、常温に冷却したりするサ
イクルを繰り返すたとえば圧力釜や保温釜などに
セラミツクヒータを接着する場合、熱伝導性、電
気絶縁性および耐熱性を併せもつた接着剤が要求
される。 従来、耐熱性接着剤としては、シリコンゴム中
にSiO2、FeO3、Al2O3などを含有させたものが
知られているが、電気絶縁性にすぐれている半
面、熱伝導率が0.86Kcal/mhr℃と低い欠点があ
る。またシリコンオイル中に95%のZnOを含有し
た接着性グリースも知られているが、上記と同様
熱伝導率は0.54kcal/mhr℃と低い欠点がある。
さらに熱伝導率が8〜10kcal/mhr℃とすぐれた
耐熱性接着剤も知られているが、金属粉末が含有
されているため比抵抗が8.4Ω/cmで電気絶縁性
が劣る欠点がある。 ところで、熱伝導性のみを向上させるにはたと
えばCu、Al、Agなどの金属粉末や炭化ケイ素
(SiC)粉末を加えればよく、たとえば合成樹脂
の熱伝導度は一般に0.1〜0.2kcal/mhr℃で、Cu
は338kcal/mhr℃、Alは194kcal/mhr℃、Fe
は61.2kcal/mhr℃、SiCは450kcal/mhrであ
る。そこで、合成樹脂に金属粉末を加えれば熱伝
導性は向上するが、しかし電気絶縁性が低下しそ
の点から使用に供し得ない。 また、難燃性無機系接着剤に電気絶縁性および
熱伝導性のすぐれた物質を混入した場合には水分
に対して弱く、湿気が通過し易くなつて電気絶縁
性が損なわれしかも長期間の使用に耐えない欠点
がある。 [発明の目的] この発明は上記の種々の欠点を除去するために
なされたもので、加熱・冷却の繰り返しサイクル
に耐え、熱伝導性、電気絶縁性および耐熱性にす
ぐれしかも長期間の使用にも耐え得る接着剤を提
供しようとするものである。 [発明の概要] この発明は熱硬化型合成樹脂中に第1図に示す
ような表面に耐食性と電気絶縁性にすぐれたセラ
ミツク層1を被覆した複合SiC粒2を含有させて
なる耐熱性接着剤である。 ここで、熱硬化型合成樹脂としては三官能性エ
ポキシ樹脂にジアミノ・ジフエニル・メタン
(DDM)
[Technical Field of the Invention] The present invention relates to a thermosetting heat-resistant adhesive having excellent thermal conductivity, electrical insulation, and heat resistance. [Technical background of the invention and its problems] Conventionally, when bonding a ceramic heater to a pressure cooker or a heat-retaining cooker that repeats cycles of heating and cooling to room temperature, thermal conductivity, electrical insulation, and heat resistance are required. An adhesive with both properties is required. Conventionally, heat-resistant adhesives containing SiO 2 , FeO 3 , Al 2 O 3, etc. in silicone rubber are known, but while they have excellent electrical insulation properties, they have a thermal conductivity of 0.86. It has the disadvantage of low Kcal/mhr℃. Adhesive grease containing 95% ZnO in silicone oil is also known, but like the above, it has the disadvantage of a low thermal conductivity of 0.54 kcal/mhr°C.
Furthermore, heat-resistant adhesives with excellent thermal conductivity of 8 to 10 kcal/mhr°C are also known, but because they contain metal powder, they have a specific resistance of 8.4 Ω/cm and have poor electrical insulation properties. By the way, to improve only the thermal conductivity, it is sufficient to add metal powder such as Cu, Al, Ag, or silicon carbide (SiC) powder.For example, the thermal conductivity of synthetic resin is generally 0.1 to 0.2 kcal/mhr℃. , Cu
is 338kcal/mhr℃, Al is 194kcal/mhr℃, Fe
is 61.2kcal/mhr℃, and SiC is 450kcal/mhr. Therefore, if metal powder is added to the synthetic resin, the thermal conductivity will be improved, but the electrical insulation properties will be reduced, making it unusable. In addition, when flame-retardant inorganic adhesives are mixed with substances with excellent electrical insulation and thermal conductivity, they are susceptible to moisture, allowing moisture to pass through easily, impairing electrical insulation properties, and causing long-term effects. There are some drawbacks that make it unusable. [Purpose of the Invention] This invention has been made to eliminate the various drawbacks mentioned above, and it has been made to withstand repeated cycles of heating and cooling, has excellent thermal conductivity, electrical insulation, and heat resistance, and can be used for a long period of time. The aim is to provide an adhesive that can withstand [Summary of the Invention] This invention provides a heat-resistant adhesive comprising composite SiC particles 2 whose surfaces are coated with a ceramic layer 1 having excellent corrosion resistance and electrical insulation properties as shown in FIG. 1 in a thermosetting synthetic resin. It is a drug. Here, as a thermosetting synthetic resin, diamino diphenyl methane (DDM) is used as a trifunctional epoxy resin.

【式】 を混合したもの(たとえば商品名:スミエポキシ
ELM−120住友化学KK)、シリコーンワニス(た
とえば商品名:TSR−117東芝シリコーンKK)、
フエノール樹脂(たとえばセメダイン−120)、ポ
リウレタン(たとえばセメダイン−700)、アクリ
ル系接着剤(たとえば商品名:ハードロツクC電
気化学KK)、ユリア樹脂、メラミン樹脂および
ポリイミド樹脂などが適用される。 SiCは熱伝導率が理論的には約450kcal/mhr℃
と極めて高く、耐熱性および耐食性にすぐれるが
電気的には通常半導性が導電性を示すので本願の
目的には不都合である。そこで本発明者らはScC
粒の表面に安定で電気絶縁性の高いセラミツクス
例えばSi3N4、Al2O3、BNなどで被覆した複合
SiC粒子を合成し使用した所、本願の効果が得ら
れた。尚、表面層物質の比率は熱伝導性と電気絶
縁性の観点から重量比で粒子の1〜50%好ましく
は5〜20%が良い。 [発明の実施例] 以下、この発明の実施例を説明する。 エポキシ樹脂、シリコンワニス、フエノール樹
脂、ポリウレタン、アクリル系樹脂などの熱硬化
型合成樹脂液に溶媒たとえばメチルエチルケトン
(MEK)を加えて適度な粘度に調整したのち表面
にSi3N4あるいはAl2O3を被覆したSiC粒子を加え
充分かきまぜて各種の耐熱性接着剤を得た。この
ようにして得た各接着剤を真空脱泡して溶媒を除
去したのち加熱硬化して1cm2の立方体をつくり熱
伝導率を測定した。その測定結果例を第1表から
第2表に示す。第1表にはエポキシ樹脂(ELM
−120)中の複合SiC粒の混合割合と熱伝導率と
の関係を示し、第2表にはシリコンワニス
(TSR−117)との関係を、それぞれ示す。 なお、表中重量はgで、混合割合は重量%で熱
伝導率はKcal/mhr℃で示している。
A mixture of [Formula] (for example, product name: Sumiepoxy
ELM-120 Sumitomo Chemical KK), silicone varnish (for example, product name: TSR-117 Toshiba Silicone KK),
Phenol resins (for example, Cemedine-120), polyurethanes (for example, Cemedine-700), acrylic adhesives (for example, trade name: Hardrock C Electrochemical KK), urea resins, melamine resins, polyimide resins, etc. are applicable. The thermal conductivity of SiC is theoretically approximately 450kcal/mhr℃
Although it has extremely high heat resistance and corrosion resistance, it is inconvenient for the purpose of the present application because semiconductivity usually exhibits electrical conductivity. Therefore, the present inventors
A composite whose grain surface is coated with stable and highly electrically insulating ceramics such as Si 3 N 4 , Al 2 O 3 , BN, etc.
When SiC particles were synthesized and used, the effects of the present application were obtained. Note that the proportion of the surface layer material is preferably 1 to 50%, preferably 5 to 20%, of the particles by weight from the viewpoint of thermal conductivity and electrical insulation. [Embodiments of the Invention] Examples of the invention will be described below. A solvent such as methyl ethyl ketone (MEK) is added to a thermosetting synthetic resin liquid such as epoxy resin, silicone varnish, phenolic resin, polyurethane, or acrylic resin to adjust the viscosity to an appropriate level, and then Si 3 N 4 or Al 2 O 3 is applied to the surface. The coated SiC particles were added and mixed thoroughly to obtain various heat-resistant adhesives. Each of the adhesives thus obtained was degassed in vacuum to remove the solvent, and then heated and cured to form a 1 cm 2 cube, and the thermal conductivity was measured. Examples of the measurement results are shown in Tables 1 and 2. Table 1 shows epoxy resin (ELM)
Table 2 shows the relationship between the mixing ratio of the composite SiC grains in (-120) and the thermal conductivity, and Table 2 shows the relationship with silicon varnish (TSR-117). In addition, the weight in the table is shown in g, the mixing ratio is shown in weight%, and the thermal conductivity is shown in Kcal/mhr°C.

【表】【table】

【表】 その他の樹脂例、フエノール樹脂、ポリウレタン
においても同様に好ましい結果がえられた。また
樹脂に溶媒を使用しないで直接例えばSi3N4を被
覆したSiC粒子を加えて充分かきまぜても接着剤
をうることができた。 一般に熱伝導率を高めるためには樹脂分を出来
るだけ少なくした方が良いが、余り少ないと使用
に耐えなくなるので、20%以上は必要である。 [発明の効果] 以上述べたようにこの発明に係る耐熱性接着剤
によれば、1従来市販されている耐熱性接着剤よ
り熱伝導性がすぐれ、2耐熱性が常時150℃以上
に保持でき、3常温から150〜200℃の加熱冷却サ
イクルに耐え、4金属粉末を加えてないので電気
伝導性がなく、5耐水性で長期の使用に耐え、し
かも6接着性がきわめて良好などの効果を奏す
る。尚、複合粒子はCDD等気相の関与する反応
を利用して比較的容易にうることができる。
[Table] Similar favorable results were obtained with other resin examples, phenolic resin, and polyurethane. It was also possible to obtain an adhesive by adding, for example, Si 3 N 4 -coated SiC particles directly to the resin without using a solvent and stirring thoroughly. Generally, in order to increase thermal conductivity, it is better to reduce the resin content as much as possible, but if it is too small, it will become unusable, so it is necessary to have a content of 20% or more. [Effects of the Invention] As described above, the heat-resistant adhesive of the present invention has (1) superior thermal conductivity than conventionally commercially available heat-resistant adhesives, and (2) can maintain heat resistance at 150°C or higher at all times. 3. It can withstand heating and cooling cycles from room temperature to 150-200℃, 4. It has no electrical conductivity because no metal powder is added, 5. It is water resistant and can withstand long-term use, and 6. It has extremely good adhesion. play. Note that composite particles can be obtained relatively easily using a reaction involving a gas phase such as CDD.

【図面の簡単な説明】[Brief explanation of the drawing]

第1図は本発明に用いる表面に絶縁性の高いセ
ラミツクスを被覆した炭化ケイ素粒を示す断面
図。 1……絶縁性の高いセラミツクス、2……炭化
ケイ素粒。
FIG. 1 is a cross-sectional view showing silicon carbide grains whose surfaces are coated with highly insulating ceramics used in the present invention. 1...Highly insulating ceramics, 2...Silicon carbide grains.

Claims (1)

【特許請求の範囲】[Claims] 1 表面に絶縁性の高いセラミツクを被覆した炭
化ケイ素粒が含有された熱硬化型合成樹脂からな
ることを特徴とする耐熱性接着剤。
1. A heat-resistant adhesive characterized by being made of a thermosetting synthetic resin containing silicon carbide particles whose surface is coated with highly insulating ceramic.
JP13121682A 1982-07-29 1982-07-29 Heat-resistant adhesive Granted JPS5922974A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP13121682A JPS5922974A (en) 1982-07-29 1982-07-29 Heat-resistant adhesive

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP13121682A JPS5922974A (en) 1982-07-29 1982-07-29 Heat-resistant adhesive

Publications (2)

Publication Number Publication Date
JPS5922974A JPS5922974A (en) 1984-02-06
JPH0322916B2 true JPH0322916B2 (en) 1991-03-27

Family

ID=15052746

Family Applications (1)

Application Number Title Priority Date Filing Date
JP13121682A Granted JPS5922974A (en) 1982-07-29 1982-07-29 Heat-resistant adhesive

Country Status (1)

Country Link
JP (1) JPS5922974A (en)

Families Citing this family (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS61157569A (en) * 1984-12-28 1986-07-17 Shin Etsu Polymer Co Ltd Thermally conductive adhesive composition
JPS6440586A (en) * 1987-08-07 1989-02-10 Hitachi Chemical Co Ltd Adhesive composition
JP2736364B2 (en) * 1990-03-23 1998-04-02 日本電信電話株式会社 High strength adhesive
JP2009230092A (en) * 2008-02-27 2009-10-08 Kyocera Corp Optical isolator module and optical element module using the same
WO2013187303A1 (en) * 2012-06-12 2013-12-19 三菱瓦斯化学株式会社 Resin composition, prepreg, metal foil-clad laminate and printed wiring board

Also Published As

Publication number Publication date
JPS5922974A (en) 1984-02-06

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