JP2001031841A - Epoxy resin composition for sealing electronic part - Google Patents

Epoxy resin composition for sealing electronic part

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Publication number
JP2001031841A
JP2001031841A JP20553999A JP20553999A JP2001031841A JP 2001031841 A JP2001031841 A JP 2001031841A JP 20553999 A JP20553999 A JP 20553999A JP 20553999 A JP20553999 A JP 20553999A JP 2001031841 A JP2001031841 A JP 2001031841A
Authority
JP
Japan
Prior art keywords
epoxy resin
coupling agent
resin composition
epoxy
component
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.)
Granted
Application number
JP20553999A
Other languages
Japanese (ja)
Other versions
JP4273374B2 (en
Inventor
Satoru Tsuchida
悟 土田
Masahiko Kosaka
正彦 小坂
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.)
Resonac Corp
Original Assignee
Hitachi Chemical 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 Hitachi Chemical Co Ltd filed Critical Hitachi Chemical Co Ltd
Priority to JP20553999A priority Critical patent/JP4273374B2/en
Publication of JP2001031841A publication Critical patent/JP2001031841A/en
Application granted granted Critical
Publication of JP4273374B2 publication Critical patent/JP4273374B2/en
Anticipated expiration legal-status Critical
Expired - Fee Related legal-status Critical Current

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  • Compositions Of Macromolecular Compounds (AREA)
  • Structures Or Materials For Encapsulating Or Coating Semiconductor Devices Or Solid State Devices (AREA)

Abstract

PROBLEM TO BE SOLVED: To obtain the subject composition excellent in adhesion with organic matters such as resist inks and various organic passivation films by including an epoxy resin, curing agent, silica powder filler and specific coupling agent. SOLUTION: This composition is obtained by including (A) an epoxy resin with >=2 epoxy groups in one molecule, (B) a curing agent where the molar ratio of the functional group in the component B to the epoxy group in the component A is 0.5-1.5, preferably 0.8-1.2, (C) 30-90 wt.% of a silica powder filler composed mainly of a spherical silica with a mean diameter of preferably <=30 μm and (D) 0.1-5 wt.%, based on the component C, of a silane coupling agent consisting of a combination of (i) a coupling agent of the formula (R is OCH3 or OC2H5) wih (ii) a silane compound selected from epoxysilane, ureidosilane, aminosilane and mercaptosilane while satisfying the weight ratio i/ii=1.0:(0.1-2.0).

Description

【発明の詳細な説明】DETAILED DESCRIPTION OF THE INVENTION

【0001】[0001]

【発明の属する技術分野】本発明は、半導体素子、LCD
等の電子部品における封止材、接着剤などに使用される
電子部品封止用エポキシ樹脂組成物に関するものであ
る。
The present invention relates to a semiconductor device, an LCD, and the like.
The present invention relates to an epoxy resin composition for sealing electronic components used for a sealing material, an adhesive, and the like in electronic components such as.

【0002】[0002]

【従来の技術】従来より、電子部品の封止材や接着剤と
して多用されているエポキシ樹脂組成物としてはフェノ
ール樹脂硬化系、無水酸硬化系、アミン硬化系、触媒硬
化系などが知られており、無機充填剤としてのシリカと
樹脂成分との界面接着を目的としてシランカップリング
剤が配合されている。シランカップリング剤の有機官能
基としては、エポキシ樹脂成分と反応する必要があるこ
とから、エポキシ基、ウレイド基、アミノ基、メルカプ
ト基などを含むシランカップリング剤が用いられてい
た。ガラス、金属、セラミックスなど無機物に対しては
上記シランカップリング剤の種類および配合量の最適化
により接着力を高めることが可能である。
2. Description of the Related Art Conventionally, epoxy resin compositions widely used as encapsulants and adhesives for electronic parts include phenol resin curing systems, acid anhydride curing systems, amine curing systems, and catalyst curing systems. In addition, a silane coupling agent is blended for the purpose of interfacial adhesion between silica as an inorganic filler and a resin component. Since the organic functional group of the silane coupling agent needs to react with the epoxy resin component, a silane coupling agent containing an epoxy group, a ureide group, an amino group, a mercapto group, or the like has been used. Adhesion to inorganic substances such as glass, metal, and ceramics can be increased by optimizing the type and amount of the silane coupling agent.

【0003】[0003]

【発明が解決しようとする課題】しかしながら、近年パ
ッケージ構造の変革が進み従来の構成要素であったシリ
コンチップ、アルミ、銅、42アロイ、窒化珪素などの
無機物の他に、ポリイミドフィルム、レジストインク、
各種有機パッシベーション膜など有機物との接着力に優
れるエポキシ樹脂組成物が要望されている。上記のシラ
ンカップリング剤ではこれら有機物との接着カを改善す
ることが困難であった。
However, in recent years, the package structure has been reformed, and in addition to inorganic components such as silicon chips, aluminum, copper, 42 alloy, silicon nitride, etc., which have been conventional components, polyimide films, resist inks, and the like.
There is a demand for epoxy resin compositions having excellent adhesion to organic substances such as various organic passivation films. With the above silane coupling agent, it was difficult to improve the adhesion to these organic substances.

【0004】[0004]

【課題を解決するための手段】本発明は、上記課題を解
決するためになされたもので、一分子中に2個以上のエ
ポキシ基を有するエポキシ樹脂とその硬化剤、およびシ
リカ粉末充填剤並びにシランカップリング剤を含むエポ
キシ樹脂組成物において、上記カップリング剤として下
記構造式(1)で表されるカップリング剤と、エポキシシ
ラン、ウレイドシラン、アミノシランおよびメルカプト
シランから選ばれるシラン化合物の1種以上を併用する
ことを特徴とする電子部品封止用エポキシ樹脂組成物に
関する。
DISCLOSURE OF THE INVENTION The present invention has been made to solve the above-mentioned problems, and an epoxy resin having two or more epoxy groups in one molecule, a curing agent thereof, a silica powder filler and In an epoxy resin composition containing a silane coupling agent, the coupling agent represented by the following structural formula (1) and one of silane compounds selected from epoxysilane, ureidosilane, aminosilane, and mercaptosilane are used as the coupling agent. The present invention relates to an epoxy resin composition for sealing electronic parts, characterized by using the above in combination.

【化2】 Embedded image

【0005】[0005]

【発明の実施の形態】本発明で用いられるエポキシ樹脂
としては一分子中に2個以上のエポキシ基を有するもで
あれば特に制限はない。これらの具体例を挙げると、ビ
スフェノールA、ビスフェノールF、ビスフェノールA
D、ビスフェノールS、水添ビスフェノールAなどのジ
グリシジルエーテル型エポキシ樹脂、オルソクレゾール
ノボラック型エポキシ樹脂を代表とするフェノール類と
アルデヒド類のノボラック樹脂をエポキシ化したもの、
フタル酸、ダイマー酸などの多塩基酸とエピクロルヒド
リンの反応により得られるグリシジルエステル型エポキ
シ樹脂、ジアミノジフェニルメタン、イソシアヌル酸な
どのポリアミンとエピクロルヒドリンの反応により得ら
れるグリシジルアミン型エポキシ樹脂、オレフィン結合
を過酢酸などの過酸により酸化して得られる線状脂肪族
エポキシ樹脂、および脂環族エポキシ樹脂などがあり、
これらを単独であるいは適宜併用して用いることができ
る。これらのエポキシ樹脂は十分に精製されたもので、
Na+、Cl−等のイオン性不純物はできるだけ少ない
ものが好ましい。
DESCRIPTION OF THE PREFERRED EMBODIMENTS The epoxy resin used in the present invention is not particularly limited as long as it has two or more epoxy groups in one molecule. Specific examples of these include bisphenol A, bisphenol F, and bisphenol A.
D, bisphenol S, diglycidyl ether type epoxy resin such as hydrogenated bisphenol A, epoxidized novolak resin of phenols and aldehydes represented by orthocresol novolak type epoxy resin,
Glycidyl ester type epoxy resin obtained by the reaction of epichlorohydrin with polybasic acids such as phthalic acid and dimer acid; glycidylamine type epoxy resin obtained by the reaction of polyamine such as diaminodiphenylmethane and isocyanuric acid with epichlorohydrin; There is a linear aliphatic epoxy resin obtained by oxidation with a peracid, and an alicyclic epoxy resin,
These can be used alone or in combination as appropriate. These epoxy resins are sufficiently refined,
It is preferable that ionic impurities such as Na + and Cl − are as small as possible.

【0006】本発明に用いられる硬化剤としては、エポ
キシ樹脂と反応して硬化可能なものであればよく特に制
限されない。この硬化剤として例えばクレゾールノボラ
ック樹脂、ビスフェノール型フェノール樹脂、アラルキ
ル型ノボラックフェノール樹脂、ヘキサヒドロ無水フタ
ル酸、テトラヒドロ無水フタル酸、無水フタル酸タイプ
の誘導体、脂肪族アミン、芳香族アミン、ジシアンジア
ミド、イミダゾール、アルミキレート、BF3錯体等が
挙げられる。これらは硬化を阻害しない範囲で単独また
は二種以上混合して使用することができる。エポキシ樹
脂と硬化剤の配合当量比(エポキシ基に対する硬化剤の
官能基のモル比)は特に限定されるものではないが、通
常好ましくは0.5〜1.5さらに好ましくは0.8〜
1.2である。本発明に用いられる充填剤としてのシリ
カ粉末としては、従来公知のものが使用できる。それら
の中でも不純物濃度が低く、平均粒径30μm以下の球
状シリカを主成分とするものが好ましい。球状シリカの
平均粒径が30μmを越えたり、また不定形シリカを主
成分とした場合には樹脂組成物の流動性が悪化するので
好ましくない。シリカ粉末の配合量は特に制限されるも
のではないが、樹脂組成物全体に対して30〜90重量
%に設定されることが好ましい。この範囲を外れると応
力歪の発生や流動性の低下を招き易くなる。
The curing agent used in the present invention is not particularly limited as long as it can be cured by reacting with an epoxy resin. As this curing agent, for example, cresol novolak resin, bisphenol type phenol resin, aralkyl type novolak phenol resin, hexahydrophthalic anhydride, tetrahydrophthalic anhydride, phthalic anhydride type derivative, aliphatic amine, aromatic amine, dicyandiamide, imidazole, aluminum Chelate, BF3 complex and the like. These can be used alone or as a mixture of two or more as long as the curing is not inhibited. The mixing equivalent ratio (molar ratio of the functional group of the curing agent to the epoxy group) of the epoxy resin and the curing agent is not particularly limited, but is usually preferably 0.5 to 1.5, and more preferably 0.8 to 1.5.
1.2. As the silica powder as a filler used in the present invention, conventionally known silica powders can be used. Among them, those containing spherical silica having a low impurity concentration and an average particle diameter of 30 μm or less as a main component are preferable. It is not preferable that the average particle diameter of the spherical silica exceeds 30 μm or that the amorphous silica is the main component, because the fluidity of the resin composition deteriorates. The blending amount of the silica powder is not particularly limited, but is preferably set to 30 to 90% by weight based on the entire resin composition. Outside this range, the occurrence of stress strain and a decrease in fluidity are likely to occur.

【0007】本発明の構造式(1)で表されるシランカッ
プリング剤は日本ユニカー(株)から販売されている。
このシランカップリング剤とともに用いられるシランカ
ップリング剤としては、有機官能基にエポキシ基、アミ
ノ基、ウレイド基、メルカプト基を有するものであれば
特に制限はなく従来から広く使用されているものでよ
く、単独または二種以上混合して使用することができ
る。これらシランカップリング剤としてはγ−グリシド
キシプロピルトリメトキシシラン、γ−グリシドキシメ
チルジエトキシシラン、γ−アミノプロピルトリェトキ
シシラン、γ−アミノプロピルメチルジエトキシシラ
ン、N−β(アミノエチル)γ−アミノプロピルトリメト
キシシラン、N−β(アミノエチル)γ−アミノプロピル
メチルジメトキシシラン、γ−メルカプトプロピルトリ
メトキシシラン、γ−メルカプトプロピルメチルジメト
キシシラン、γ−ウレイドプロピルトリエトキシシラン
等が例示される。カップリング剤の配合割合は、シリカ
粉末に対して0.1〜5重量%の範囲に設定することが
好ましく、またカップリング剤の併用重量比率は、構造
式(1)のカップリング剤:併用カップリング剤=1.
0:0.1〜2.0が無機物、有機物に対する接着力の
バランスがとれ好ましい。
The silane coupling agent represented by the structural formula (1) of the present invention is sold by Nippon Unicar Co., Ltd.
The silane coupling agent used together with the silane coupling agent is not particularly limited as long as it has an epoxy group, an amino group, a ureide group, or a mercapto group in the organic functional group, and may be a conventionally widely used one. , Or a mixture of two or more. These silane coupling agents include γ-glycidoxypropyltrimethoxysilane, γ-glycidoxymethyldiethoxysilane, γ-aminopropyltriethoxysilane, γ-aminopropylmethyldiethoxysilane, N-β (aminoethyl ) γ-aminopropyltrimethoxysilane, N-β (aminoethyl) γ-aminopropylmethyldimethoxysilane, γ-mercaptopropyltrimethoxysilane, γ-mercaptopropylmethyldimethoxysilane, γ-ureidopropyltriethoxysilane, etc. Is done. The compounding ratio of the coupling agent is preferably set in the range of 0.1 to 5% by weight with respect to the silica powder, and the combined weight ratio of the coupling agent is the coupling agent of the structural formula (1): Coupling agent = 1.
0: 0.1 to 2.0 is preferable because the balance of the adhesive strength to inorganic substances and organic substances can be obtained.

【0008】なお、本発明のエポキシ樹脂組成物には上
記成分以外に、必要に応じて他の添加剤を適宜配合する
ことができる。前記の添加剤としては難燃剤、触媒、希
釈剤、着色剤、レベリング剤、消泡剤、イオントラップ
剤、溶剤等が挙げられる。上記難燃剤としてはブロム化
エポキシ樹脂、三酸化アンチモン、四酸化アンチモン、
五酸化アンチモン、リン系化合物、金属水酸化物等が挙
げられ、単独でもしくは2種以上併せて用いられる。本
発明のエポキシ樹脂組成物は、液状組成物の場合通常各
成分、添加剤等を三本ロール、擂潰機等を使って分散混
練して製造される。また固形組成物の場合には各成分混
合後、ミキシングロール、押出機等の混練機により加熱
状態で溶融混合する。つぎに、これを冷却・粉砕したの
ち必要に応じて打錠するこよにより目的とする固形組成
物を製造することができる。
[0008] In addition to the above components, the epoxy resin composition of the present invention may optionally contain other additives as necessary. Examples of the additives include a flame retardant, a catalyst, a diluent, a coloring agent, a leveling agent, an antifoaming agent, an ion trapping agent, and a solvent. As the flame retardant, brominated epoxy resin, antimony trioxide, antimony tetroxide,
Antimony pentoxide, phosphorus compounds, metal hydroxides and the like can be mentioned, and these are used alone or in combination of two or more. In the case of a liquid composition, the epoxy resin composition of the present invention is usually produced by dispersing and kneading components, additives and the like using a three-roll mill, a crusher or the like. In the case of a solid composition, after mixing each component, it is melted and mixed in a heated state by a kneader such as a mixing roll or an extruder. Next, after cooling and pulverizing the mixture, tableting is performed as necessary to produce a target solid composition.

【0009】[0009]

【実施例】以下実施例によって本発明をさらに具体的に
説明するが、本発明はこれらの実施例に限定されるもの
ではない。表1に従って各原材料を配合し、3本ロール
にて常温で10分間混練分散後、1Torrの真空度で
10分間真空脱泡して液状エポキシ樹脂組成物を得た。
次いで、アルミニウム箔あるいはポリイミドフィルムの
片面に上記の樹脂組成物を塗布し150℃で4時間硬化
し、試験片を作製した。この試験片をオートグラフAG
S−500A型(株.島津製作所製)を用いて30mm/
minの速度でアルミニウム箔あるいはポリイミドフィ
ルムを垂直にピールすることにより、エポキシ硬化物に
対するピール強さ(接着強さ)を測定した。またPCT
(121℃ 2atm 100%RH)72h,168h,
240h処理した後のピール強さを測定した。結果を表
2に示す。実施例1〜4のエポキシ樹脂組成物は無機物
(アルミ)および有機物(ポリイミド)の両方に対して優れ
た接着力を示すことが分かる。一方、比較例1の樹脂組
成物は構造式(1)のカップリング剤のみ配合のため有機
物には優れた接着力を示すが、無機物に対しては接着が
悪い。比較例2〜5は従来からのシランカップリング剤
を配合しているため無機物に対しては良好な接着を示す
が有機物との接着が悪い。
EXAMPLES The present invention will be described in more detail with reference to the following examples, but the present invention is not limited to these examples. Each raw material was blended according to Table 1, kneaded and dispersed with a three-roll mill at room temperature for 10 minutes, and then vacuum degassed at 1 Torr vacuum for 10 minutes to obtain a liquid epoxy resin composition.
Next, the above resin composition was applied to one side of an aluminum foil or a polyimide film and cured at 150 ° C. for 4 hours to prepare a test piece. Autograph AG
30mm / S-500A type (manufactured by Shimadzu Corporation)
The peel strength (adhesion strength) to the epoxy cured product was measured by vertically peeling the aluminum foil or the polyimide film at a speed of min. Also PCT
(121 ° C 2atm 100% RH) 72h, 168h,
The peel strength after 240 hours of treatment was measured. Table 2 shows the results. The epoxy resin compositions of Examples 1 to 4 are inorganic
It can be seen that it exhibits excellent adhesion to both (aluminum) and organic substances (polyimide). On the other hand, since the resin composition of Comparative Example 1 contains only the coupling agent of the structural formula (1), it exhibits excellent adhesion to organic substances, but has poor adhesion to inorganic substances. Comparative Examples 2 to 5 show good adhesion to inorganic substances, but poor adhesion to organic substances, because they contain a conventional silane coupling agent.

【0010】[0010]

【表1】 [Table 1]

【0011】[0011]

【表2】 [Table 2]

【0012】[0012]

【発明の効果】本発明によるエポキシ樹脂組成物は、吸
湿後においても無機物、有機物と十分な接着力を有し耐
湿信頼性に優れた電子部品を提供することが可能となっ
た。
As described above, the epoxy resin composition of the present invention can provide an electronic component having sufficient adhesion to inorganic and organic substances even after absorbing moisture and having excellent moisture resistance reliability.

───────────────────────────────────────────────────── フロントページの続き (51)Int.Cl.7 識別記号 FI テーマコート゛(参考) H01L 23/29 H01L 23/30 R 23/31 Fターム(参考) 4J002 CC042 CC052 CD011 CD021 CD051 CD061 CD081 CD131 DJ017 EL136 EN016 EN056 EQ006 EU116 EU198 EX059 EX078 EX079 EX089 EZ006 FD017 FD142 FD146 GQ05 4M109 AA01 BA03 CA05 EA03 EB02 EB04 EB06 EB07 EB08 EB13 EB16 EB18 EC09 ──────────────────────────────────────────────────続 き Continued on the front page (51) Int.Cl. 7 Identification symbol FI Theme coat ゛ (Reference) H01L 23/29 H01L 23/30 R 23/31 F term (Reference) 4J002 CC042 CC052 CD011 CD021 CD051 CD061 CD081 CD131 DJ017 EL136 EN016 EN056 EQ006 EU116 EU198 EX059 EX078 EX079 EX089 EZ006 FD017 FD142 FD146 GQ05 4M109 AA01 BA03 CA05 EA03 EB02 EB04 EB06 EB07 EB08 EB13 EB16 EB18 EC09

Claims (1)

【特許請求の範囲】[Claims] 【請求項1】一分子中に2個以上のエポキシ基を有する
エポキシ樹脂とその硬化剤、およびシリカ粉末充填剤並
びにシランカップリング剤を含むエポキシ樹脂組成物に
おいて、上記カップリング剤として下記構造式(1)で表
されるカップリング剤と、エポキシシラン、ウレイドシ
ラン、アミノシランおよびメルカプトシランから選ばれ
るシラン化合物の1種以上を併用することを特徴とする
電子部品封止用エポキシ樹脂組成物。 【化1】
An epoxy resin composition comprising an epoxy resin having two or more epoxy groups in one molecule, a curing agent thereof, a silica powder filler and a silane coupling agent, wherein the coupling agent has the following structural formula: An epoxy resin composition for sealing electronic components, comprising a combination of the coupling agent represented by (1) and one or more silane compounds selected from epoxysilane, ureidosilane, aminosilane and mercaptosilane. Embedded image
JP20553999A 1999-07-21 1999-07-21 Epoxy resin composition for sealing electronic parts Expired - Fee Related JP4273374B2 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP20553999A JP4273374B2 (en) 1999-07-21 1999-07-21 Epoxy resin composition for sealing electronic parts

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP20553999A JP4273374B2 (en) 1999-07-21 1999-07-21 Epoxy resin composition for sealing electronic parts

Publications (2)

Publication Number Publication Date
JP2001031841A true JP2001031841A (en) 2001-02-06
JP4273374B2 JP4273374B2 (en) 2009-06-03

Family

ID=16508577

Family Applications (1)

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Country Status (1)

Country Link
JP (1) JP4273374B2 (en)

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2002097341A (en) * 2000-09-20 2002-04-02 Sumitomo Bakelite Co Ltd Epoxy resin composition and semiconductor device
JP2002275354A (en) * 2001-03-21 2002-09-25 Toray Ind Inc Epoxy resin composition for sealing semiconductor, and semiconductor device
JP2003105169A (en) * 2001-09-28 2003-04-09 Toray Ind Inc Epoxy resin composition and semiconductor device
EP1469022A1 (en) * 2002-10-28 2004-10-20 Nikko Materials Co., Ltd. Solid silane coupling agent composition, process for producing the same, and resin composition containing the same
WO2005080502A1 (en) * 2004-02-24 2005-09-01 Matsushita Electric Works, Ltd. Liquid epoxy resin composition for underfill and semiconductor device encapsulated with the composition
JP2017043560A (en) * 2015-08-27 2017-03-02 株式会社クラレ Nitrogen-containing organic silicon compound and resin composition

Cited By (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2002097341A (en) * 2000-09-20 2002-04-02 Sumitomo Bakelite Co Ltd Epoxy resin composition and semiconductor device
JP2002275354A (en) * 2001-03-21 2002-09-25 Toray Ind Inc Epoxy resin composition for sealing semiconductor, and semiconductor device
JP2003105169A (en) * 2001-09-28 2003-04-09 Toray Ind Inc Epoxy resin composition and semiconductor device
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