JP2000103939A5

JP2000103939A5 -

Info

Publication number: JP2000103939A5
Application number: JP1998276344A
Authority: JP
Filing date: 1998-09-30
Publication date: 2004-12-24
Anticipated expiration: 2018-09-30

Description

【０００５】
すなわち、本発明は、
（１）（Ａ）１分子中に２個以上のエポキシ基を有するエポキシ樹脂、（Ｂ）１分子中に２個以上のフェノール性水酸基を有する化合物、（Ｃ）主鎖骨格中に次式（Ｉ）及び／又は次式（II）を繰り返し単位として含む環状ホスファゼン化合物、（Ｄ）無機充填剤、を必須成分とし、（Ｄ）成分の含有量が成形材料全体に対して７０重量％以上であることを特徴とする封止用エポキシ樹脂成形材料、
【化６】

（ここで、式（Ｉ）中のｍは１〜１０の整数で、Ｒ¹〜Ｒ⁴は置換基を有しても良い炭素数１〜１２のアルキル基及びアリール基から選ばれ、全て同一でも異なっていても良いが少なくとも１つは水酸基を有する基であり、Ａは炭素数１〜４のアルキレン基又はアリレン基を示す。式（II）中のｎは１〜１０の整数で、Ｒ⁵〜Ｒ⁸は置換基を有しても良い炭素数１〜４のアルキル基又はアリール基から選ばれ、全て同一でも異なっていても良く、Ａは炭素数１〜４のアルキレン基又はアリレン基を示す。）
（２）（Ａ）１分子中に２個以上のエポキシ基を有するエポキシ樹脂、（Ｂ）１分子中に２個以上のフェノール性水酸基を有する化合物、（Ｃ）主鎖骨格中に次式（III）及び／又は次式（IV）を繰り返し単位として含む環状ホスファゼン化合物、（Ｄ）無機充填剤、を必須成分とし、（Ｄ）成分の含有量が成形材料全体に対して７０重量％以上であることを特徴とする封止用エポキシ樹脂成形材料、
【化７】

（ここで、式（III）中のｍは１〜１０の整数で、Ｒ¹〜Ｒ⁴は置換基を有しても良い炭素数１〜１２のアルキル基及びアリール基から選ばれ、全て同一でも異なっていても良いが少なくとも１つは水酸基を有する基であり、Ａは炭素数１〜４のアルキレン基又はアリレン基を示す。式（IV）中のｎは１〜１０の整数で、Ｒ⁵〜Ｒ⁸は置換基を有しても良い炭素数１〜１２のアルキル基又はアリール基から選ばれ、全て同一でも異なっていても良く、Ａは炭素数１〜４のアルキレン基又はアリレン基を示す。）
（３）（Ｃ）成分が主鎖骨格中に次式（Ｖ）及び／又は次式（VI）を繰り返し単位として含む環状ホスファゼン化合物であることを特徴とする上記（１）記載の封止用エポキシ樹脂成形材料、
【化８】

（ここで、式（Ｖ）中のｍは１〜１０の整数で、Ｒ⁹〜Ｒ¹²は水素、炭素数１〜４のアルキル基、アルコキシル基、アリール基、水酸基、アミノ基、エポキシ基から選ばれ、全て同一でも異なっていても良いが、少なくとも１つは水酸基を示す。式（VI）中のｎは１〜１０の整数で、Ｒ¹³〜Ｒ¹⁶は水素、炭素数１〜４のアルキル基、アルコキシル基、アリール基、水酸基、アミノ基、エポキシ基から選ばれ、全て同一でも異なっていても良い。）
（４）（Ｃ）成分が主鎖骨格中に次式（VII）及び／又は（VIII）を繰り返し単位として含む環状ホスファゼン化合物であることを特徴とする上記（２）記載の封止用エポキシ樹脂成形材料、
【化９】

（ここで、式（VII）中のｍは１〜１０の整数で、Ｒ⁹〜Ｒ¹²は水素、炭素数１〜４のアルキル基、アルコキシル基、アリール基、水酸基、アミノ基、エポキシ基から選ばれ、全て同一でも異なっていても良いが、少なくとも１つは水酸基を示す。式（VIII）中のｎは１〜１０の整数で、Ｒ¹³〜Ｒ¹⁶は水素、炭素数１〜４のアルキル基、アルコキシル基、アリール基、水酸基、アミノ基、エポキシ基から選ばれ、全て同一でも異なっていても良い。）
（５）（Ｃ）成分の主鎖骨格中に含まれる式（Ｉ）〜式（IV）中のＲ¹〜Ｒ⁴のうち１個がヒドロキシフェニル基、他の３個がフェニル基、Ｒ⁵〜Ｒ⁸の全てがフェニル基、Ａがフェニレン基である上記（１）又は上記（２）記載の電子部品封止用エポキシ樹脂成形材料、
（６）（Ｃ）成分の主鎖骨格中に含まれる式（Ｉ）〜式（VIII）のモル比（ｍ／ｎ）が１／０〜１／４である上記（１）〜上記（５）記載のいずれかの封止用エポキシ樹脂成形材料、
（７）（Ｃ）成分の含有量は無機充填剤（Ｄ）を除く配合成分の合計量に対して燐原子の量が０．２〜５．０重量％となる量である上記（１）〜上記（６）記載のいずれかの封止用エポキシ樹脂成形材料、
（８）（Ａ）成分が次式（IX）で示されるエポキシ樹脂、
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、
ビスフェノールＡ、ビスフェノールＦ、ビスフェノールＳ、アルキル置換又は非置換のビフェノールなどのジグリシジルエーテル、
グリシジルアミン型エポキシ樹脂、
ジシクロペンタジエンとフェノール類の共縮合樹脂のエポキシ化物、
トリメチロールプロパン型エポキシ樹脂、
テルペン変性エポキシ樹脂、
線状脂肪族エポキシ樹脂、
及び脂環族エポキシ樹脂の何れかを少なくとも含むことを特徴とする上記（１）〜上記（７）記載のいずれかの封止用エポキシ樹脂成形材料、
【化１０】

（ここで、ｎは０〜３を示し、Ｒ¹⁷〜Ｒ²⁰は水素、炭素数１〜１０のアルキル基、アルコキシル基、アリール基及びアラルキル基から選ばれ、全て同一でも異なっても良い。）
（９）（Ｂ）成分が、フェノール類又はナフトール類とアルデヒド類とを酸性触媒下で縮合又は共縮合させて得られる樹脂、
ポリパラビニルフェノール樹脂、
フェノール類とジメトキシパラキシレンから合成されるキシリレン基を有するフェノール・アラルキル樹脂の何れかを少なくとも含む上記（１）〜上記（８）記載のいずれかの電子部品封止用エポキシ樹脂成形材料、
（１０）更にカップリング剤を含む上記（１）〜上記（９）記載のいずれかの封止用エポキシ樹脂成形材料、
（１１）上記（１）〜上記（１０）記載のいずれかの封止用エポキシ樹脂成形材料により封止された素子を備える電子部品装置、
である。[0005]
That is, the present invention
(1) (A) an epoxy resin having two or more epoxy groups in one molecule, (B) a compound having two or more phenolic hydroxyl groups in one molecule, (C) The cyclic phosphazene compound which contains I) and / or the following formula (II) as a repeating unit, (D) an inorganic filler is an essential component, and the content of the component (D) is 70% by weight or more based on the whole molding material An epoxy resin molding material for sealing, characterized in that
[Chemical formula 6]

(Here, m in the formula (I) is an integer of 1 to 10, and R ^{1 to} R ⁴ are selected from an alkyl group having 1 to 12 carbon atoms which may have a substituent and an aryl group, all identical) However, it may be different, but at least one is a group having a hydroxyl group, and A represents an alkylene group having 1 to 4 carbon atoms or an allylene group, and n in the formula (II) is an integer of 1 to 10, R ^{5 to} R ⁸ are selected from an alkyl group having 1 to 4 carbon atoms which may have a substituent or an aryl group, which may be all identical or different, and A is an alkylene group having 1 to 4 carbon atoms or an allylene group Indicate
(2) (A) an epoxy resin having two or more epoxy groups in one molecule, (B) a compound having two or more phenolic hydroxyl groups in one molecule, (C) A cyclic phosphazene compound containing as a repeating unit III) and / or the following formula (IV), (D) an inorganic filler as an essential component, and the content of the component (D) is 70% by weight or more based on the entire molding material An epoxy resin molding material for sealing, characterized in that
[Chemical formula 7]

(Here, m in the formula (III) is an integer of 1 to 10, and R ^{1 to} R ⁴ are selected from an alkyl group having 1 to 12 carbon atoms which may have a substituent and an aryl group, all identical) However, it may be different, but at least one is a group having a hydroxyl group, and A represents an alkylene group having 1 to 4 carbon atoms or an arylene group, n in the formula (IV) is an integer of 1 to 10, R ^{5 to} R ⁸ are selected from an alkyl or aryl group having 1 to 12 carbon atoms which may have a substituent, and may be all identical or different, and A is an alkylene or arylene group having 1 to 4 carbon atoms Indicate
(3) The sealing composition according to the above (1), wherein the component (C) is a cyclic phosphazene compound containing the following formula (V) and / or the following formula (VI) as a repeating unit in the main chain skeleton. Epoxy resin molding material,
[Image 8]

(Wherein m in the formula (V) is an integer of 1 to 10, R ^{9 to} R ¹² are hydrogen, an alkyl group having 1 to 4 carbon atoms, an alkoxyl group, an aryl group, a hydroxyl group, an amino group, an epoxy group It is selected and all of them may be the same or different, but at least one represents a hydroxyl group, n in the formula (VI) is an integer of 1 to 10, R ^{13 to} R ¹⁶ are hydrogen and has 1 to 4 carbon atoms It is selected from an alkyl group, an alkoxyl group, an aryl group, a hydroxyl group, an amino group and an epoxy group, and may be all the same or different.)
(4) The epoxy resin for sealing according to the above (2), wherein the component (C) is a cyclic phosphazene compound containing the following formula (VII) and / or (VIII) as a repeating unit in the main chain skeleton: Molding material,
Embedded image

(Wherein m in the formula (VII) is an integer of 1 to 10, and R ^{9 to} R ¹² are hydrogen, an alkyl group having 1 to 4 carbon atoms, an alkoxyl group, an aryl group, a hydroxyl group, an amino group or an epoxy group It is selected and all of them may be the same or different, but at least one represents a hydroxyl group, n in the formula (VIII) is an integer of 1 to 10, R ^{13 to} R ¹⁶ are hydrogen, and have 1 to 4 carbon atoms It is selected from an alkyl group, an alkoxyl group, an aryl group, a hydroxyl group, an amino group and an epoxy group, and may be all the same or different.)
(5) ^One of R ^{1 to} R ^{4 in} the formulas (I) to (IV) contained in the main chain skeleton of the component (C) is a hydroxyphenyl group, and the other three are a phenyl group, R ⁵ all phenyl groups to R ^8, the a is a phenylene group (1) or (2) an epoxy resin molding material for electronic part sealing, wherein,
(6) The above (1) to (5) wherein the molar ratio (m / n) of the formula (I) to the formula (VIII) contained in the main chain skeleton of the (C) component is 1/0 to 1/4. A sealing epoxy resin molding material according to any of the above,
(7) The content of the component (C) is an amount such that the amount of phosphorus atoms is 0.2 to 5.0% by weight based on the total amount of the components excluding the inorganic filler (D). -Epoxy resin molding material for sealing according to any one of the above (6),
(8) Epoxy resin whose component (A) is represented by the following formula (IX) :
Epoxidized novolak resin of phenols and aldehydes,
Diglycidyl ethers such as bisphenol A, bisphenol F, bisphenol S, alkyl-substituted or unsubstituted biphenols,
Glycidylamine type epoxy resin,
Epoxide of co-condensed resin of dicyclopentadiene and phenols,
Trimethylolpropane type epoxy resin,
Terpene modified epoxy resin,
Linear aliphatic epoxy resin,
And the sealing epoxy resin molding material according to any one of the above (1) to (7), which contains at least one of an alicyclic epoxy resin,
[Image 10]

(Here, n represents 0 to 3, and R ^{17 to} R ²⁰ are selected from hydrogen, an alkyl group having 1 to 10 carbon atoms, an alkoxyl group, an aryl group and an aralkyl group, and they may be all the same or different.)
(9) A resin obtained by component (B) by condensation or cocondensation of phenols or naphthols with aldehydes under an acidic catalyst,
Poly para vinyl phenol resin,
The epoxy resin molding material according to any one of the above (1) to (8) according to any one of the above (1) to (8), which contains at least one of phenols and phenol / aralkyl resins having xylylene group synthesized from dimethoxyparaxylene.
(10) The epoxy resin molding material for sealing according to any one of the above (1) to (9), further containing a coupling agent,
(11) An electronic component device comprising an element sealed by the sealing epoxy resin molding material according to any one of (1) to ( 10 ) above,
It is.

Claims

(A) an epoxy resin having two or more epoxy groups in one molecule,
(B) a compound having two or more phenolic hydroxyl groups in one molecule,
(C) A cyclic phosphazene compound comprising the following formula (I) and / or the following formula (II) as a repeating unit in the main chain skeleton,

(Here, m in the formula (I) is an integer of 1 to 10, and R ^{1 to} R ⁴ are selected from an alkyl group having 1 to 12 carbon atoms which may have a substituent and an aryl group, all identical) However, it may be different, but at least one is a group having a hydroxyl group, and A represents an alkylene group having 1 to 4 carbon atoms or an allylene group, and n in the formula (II) is an integer of 1 to 10, R ^{5 to} R ⁸ are selected from an alkyl or aryl group having 1 to 12 carbon atoms which may have a substituent, and may be all identical or different, and A is an alkylene or arylene group having 1 to 4 carbon atoms Indicate
(D) Inorganic filler,
An epoxy resin molding material for sealing, characterized in that the content of the component (D) is 70% by weight or more based on the entire molding material.

(A) an epoxy resin having two or more epoxy groups in one molecule,
(B) a compound having two or more phenolic hydroxyl groups in one molecule,
(C) A cyclic phosphazene compound comprising the following formula (III) and / or the following formula (IV) as a repeating unit in the main chain skeleton,

(Here, m in the formula (III) is an integer of 1 to 10, and R ^{1 to} R ⁴ are selected from an alkyl group having 1 to 12 carbon atoms which may have a substituent and an aryl group, all identical) However, it may be different, but at least one is a group having a hydroxyl group, and A represents an alkylene group having 1 to 4 carbon atoms or an arylene group, n in the formula (IV) is an integer of 1 to 10, R ^{5 to} R ⁸ are selected from an alkyl or aryl group having 1 to 12 carbon atoms which may have a substituent, and may be all identical or different, and A is an alkylene or arylene group having 1 to 4 carbon atoms Indicate
(D) Inorganic filler,
An epoxy resin molding material for sealing, characterized in that the content of the component (D) is 70% by weight or more based on the entire molding material.

The epoxy resin molding material for sealing according to claim 1, wherein the component (C) is a cyclic phosphazene compound containing the following formula (V) and / or the following formula (VI) as a repeating unit in the main chain skeleton. .

(Wherein m in the formula (V) is an integer of 1 to 10, R ^{9 to} R ¹² are hydrogen, an alkyl group having 1 to 4 carbon atoms, an alkoxyl group, an aryl group, a hydroxyl group, an amino group, an epoxy group It is selected and all of them may be the same or different, but at least one represents a hydroxyl group, n in the formula (VI) is an integer of 1 to 10, R ^{13 to} R ¹⁶ are hydrogen and has 1 to 4 carbon atoms It is selected from an alkyl group, an alkoxyl group, an aryl group, a hydroxyl group, an amino group and an epoxy group, and may be all the same or different.)

The epoxy resin molding material for sealing according to claim 2, wherein the component (C) is a cyclic phosphazene compound containing the following formula (VII) and / or the following formula (VIII) as a repeating unit in the main chain skeleton. .

(Wherein m in the formula (VII) is an integer of 1 to 10, and R ^{9 to} R ¹² are hydrogen, an alkyl group having 1 to 4 carbon atoms, an alkoxyl group, an aryl group, a hydroxyl group, an amino group or an epoxy group It is selected and all of them may be the same or different, but at least one represents a hydroxyl group, n in the formula (VIII) is an integer of 1 to 10, R ^{13 to} R ¹⁶ are hydrogen, and have 1 to 4 carbon atoms It is selected from an alkyl group, an alkoxyl group, an aryl group, a hydroxyl group, an amino group and an epoxy group, and may be all the same or different.)

^One of R ^{1 to} R ^{4 in} the formulas (I) to (IV) contained in the main chain skeleton of the component (C) is a hydroxyphenyl group, and the other three are a phenyl group, R ^{5 to} R ⁸ The epoxy resin molding material for sealing according to claim 1 or 2, wherein all of the groups are a phenyl group and A is a phenylene group.

The molar ratio (m / n) of the formula (I) to the formula (VIII) contained in the main chain skeleton of the component (C) is 1/0 to 1/4. Epoxy resin molding material for any sealing.

The content of the component (C) is an amount such that the amount of phosphorus atoms is 0.2 to 5.0% by weight based on the total amount of the components excluding the inorganic filler (D). The epoxy resin molding material for sealing in any one of each description.

An epoxy resin of which the component (A) is represented by the following formula (IX) :
Epoxidized novolak resin of phenols and aldehydes,
Diglycidyl ethers such as bisphenol A, bisphenol F, bisphenol S, alkyl-substituted or unsubstituted biphenols,
Glycidylamine type epoxy resin,
Epoxide of co-condensed resin of dicyclopentadiene and phenols,
Trimethylolpropane type epoxy resin,
Terpene modified epoxy resin,
Linear aliphatic epoxy resin,
The epoxy resin molding material for sealing according to any one of claims 1 to 7, which contains at least one of an alicyclic epoxy resin.

(Here, n represents 0 to 3, and R ^{17 to} R ²⁰ are selected from hydrogen, an alkyl group having 1 to 10 carbon atoms, an alkoxyl group, an aryl group and an aralkyl group, and they may be all the same or different.)

(B) A resin obtained by condensation or cocondensation of phenols or naphthols with aldehydes under an acidic catalyst,
Poly para vinyl phenol resin,
9. The epoxy resin molding material for electronic component sealing according to any one of claims 1 to 8, containing at least one of phenols and phenol-aralkyl resins having a xylylene group synthesized from dimethoxyparaxylene.

The epoxy resin molding material for sealing according to any one of claims 1 to 9, further comprising a coupling agent.

An electronic component device comprising an element sealed with the sealing epoxy resin molding material according to any one of claims 1 to 10 .