JPH0985891A - Manufacture of laminated board, manufacture of prepreg for the laminated board and glass woven fabric for the laminated board - Google Patents
Manufacture of laminated board, manufacture of prepreg for the laminated board and glass woven fabric for the laminated boardInfo
- Publication number
- JPH0985891A JPH0985891A JP24604995A JP24604995A JPH0985891A JP H0985891 A JPH0985891 A JP H0985891A JP 24604995 A JP24604995 A JP 24604995A JP 24604995 A JP24604995 A JP 24604995A JP H0985891 A JPH0985891 A JP H0985891A
- Authority
- JP
- Japan
- Prior art keywords
- glass
- woven fabric
- glass woven
- thermal expansion
- coupling agent
- 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.)
- Pending
Links
Classifications
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
- H05K1/00—Printed circuits
- H05K1/02—Details
- H05K1/03—Use of materials for the substrate
- H05K1/0313—Organic insulating material
- H05K1/0353—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement
- H05K1/0366—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement reinforced, e.g. by fibres, fabrics
Abstract
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、プリント配線の基
板として適した低熱膨張の積層板の製造法、積層板用プ
リプレグの製造法、ならびにこれらの製造に使用する積
層板用ガラス織布に関する。本発明において、積層板と
は、表面に金属箔を一体に貼り付けた金属箔張り積層
板、内層にプリント配線を有する多層板をその概念に含
む。また、積層板用プリプレグとは、これを重ねて加熱
加圧成形して積層板を製造する用途に供するもののほ
か、プリント配線板同士の間に介在させて、加熱加圧成
形により多層板を製造する用途に供するものをその概念
に含む。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method for producing a laminate having a low thermal expansion suitable as a substrate for printed wiring, a method for producing a prepreg for a laminate, and a glass woven fabric for a laminate used in the production thereof. In the present invention, the concept of the laminated plate includes a metal foil-clad laminated plate having a surface integrally bonded with a metal foil, and a multilayer plate having a printed wiring as an inner layer. In addition, laminated prepregs are used for manufacturing laminated boards by stacking them and heating and pressurizing them, or by interposing between printed wiring boards and manufacturing multilayer boards by heating and pressurizing. The concept includes things to be used for.
【０００２】[0002]
【従来の技術】近年、電子機器に使用される半導体パッ
ケージは、薄型化によりその熱膨張率が小さくなってい
る。そのため、当該パッケージを実装するプリント配線
の基板に、低熱膨張化が強く要求されている。また、液
晶ディスプレイとそのドライバ基板の関係においては、
ディスプレイガラスとドライバ基板の熱膨張率の違いに
起因して生じる両者の寸法変化の差が、ディスプレイの
大型化に伴って著しくなり、通常のガラスエポキシ基板
では対応が難しくなっている。すなわち、前記寸法変化
の差から生じる応力が、ディスプレイガラスとドライバ
基板を接続するＴＡＢに集中してその断線を招く問題か
ら、やはり、プリント配線の基板の低熱膨張化が強く望
まれている。従来、ＯＡ機器や産業機器、計測機器な
ど、高信頼性が必要とされる機器に組み込まれているプ
リント配線の基板には、ＮＥＭＡ規格ＦＲ−４（ガラス
織布エポキシ樹脂積層板）が一般的に使用されている。
さらに高度な機器においては、ＮＥＭＡ規格ＧＰＹ（ガ
ラス織布ポリイミド及びガラス織布ＢＴ樹脂積層板）が
使用されている。いずれも、ガラス織布を構成するガラ
ス繊維にはＥガラス（熱膨張率：５．６ｐｐｍ／℃）を
使用しているために、基板の熱膨張率は１２〜１５ｐｐ
ｍ／℃と大きな値であった。一方、プリント配線の低熱
膨張基板として、Ｓガラス（熱膨張率：２．４ｐｐｍ／
℃，代表的組成ＳｉＯ2：６５％，Ａｌ2Ｏ3：２５％，
ＭｇＯ：１０％）やＤガラス（熱膨張率：３．１ｐｐｍ
／℃）、Ｑガラス（熱膨張率：０．５ｐｐｍ／℃）など
低熱膨張のガラス繊維で構成したガラス織布を使用した
エポキシ樹脂積層板やポリイミド積層板が開発されてい
る。2. Description of the Related Art In recent years, semiconductor packages used in electronic equipment have become smaller in thermal expansion coefficient due to the reduction in thickness. For this reason, there is a strong demand for low thermal expansion of the printed wiring board on which the package is mounted. Also, regarding the relationship between the liquid crystal display and its driver board,
The difference in the dimensional changes between the display glass and the driver substrate caused by the difference in the coefficient of thermal expansion between the display glass and the driver substrate becomes remarkable with the increase in size of the display, and it is difficult to cope with this with a normal glass epoxy substrate. That is, the stress caused by the difference in the dimensional change is concentrated in the TAB that connects the display glass and the driver substrate and causes a disconnection, so that it is strongly desired to reduce the thermal expansion of the substrate for the printed wiring. Conventionally, NEMA standard FR-4 (glass woven epoxy resin laminated board) is generally used for printed wiring boards incorporated in equipment requiring high reliability such as OA equipment, industrial equipment, and measurement equipment. Is used for.
In more advanced equipment, NEMA standard GPY (glass woven polyimide and glass woven BT resin laminate) is used. In both cases, since E glass (coefficient of thermal expansion: 5.6 ppm / ° C.) is used for the glass fibers constituting the glass woven cloth, the coefficient of thermal expansion of the substrate is 12 to 15 pp.
It was a large value of m / ° C. On the other hand, S glass (coefficient of thermal expansion: 2.4 ppm /
℃, typical composition SiO 2 : 65%, Al 2 O 3 : 25%,
MgO: 10%) and D glass (coefficient of thermal expansion: 3.1 ppm)
/ ° C.), Q glass (coefficient of thermal expansion: 0.5 ppm / ° C.), epoxy resin laminates and polyimide laminates using glass woven fabrics made of low thermal expansion glass fibers have been developed.
【０００３】プリント配線の基板となる積層板に使用す
るガラス織布は、ＭＩＬ規格＃７１９５タイプ（厚み１
８０μｍ）、＃２１１６タイプ（厚み１００μｍ）、＃
１０６タイプ（厚み６０μｍ）が一般的であり、ガラス
織布に含浸した樹脂とガラス繊維の界面の接着性を向上
させるために、ガラス織布をカップリング剤で処理して
いる。カップリング剤は、γ−アミノフェニル−トリメ
トキシシラン、Ｎ−（βアミノエチル）−γ−アミノプ
ロピルトリメトキシシラン等のアミノシラン系カップリ
ング剤、ビニルトリエトキシシラン、ビニル−トリス
（２−メトキシ−エトキシ）シラン、γ−メタクリロキ
シプロピルトリメトキシシラン等のカチオニックシラン
系カップリング剤や、β−（３，４−エポキシシクロヘ
キシル）エチルトリメトキシシラン、γ−グリシドキシ
−プロピルトリメトキシシラン等のエポキシシラン系カ
ップリング剤等である。このうち、ガラス織布に含浸す
る熱硬化性樹脂がエポキシ樹脂の場合には、カチオニッ
クシラン系カップリング剤を用いるのが一般的である。The glass woven fabric used for the laminated board which is the substrate of the printed wiring is MIL standard # 7195 type (thickness 1
80 μm), # 2116 type (100 μm thickness), #
The 106 type (thickness 60 μm) is generally used, and the glass woven cloth is treated with a coupling agent in order to improve the adhesiveness at the interface between the resin impregnated in the glass woven cloth and the glass fiber. Coupling agents include aminosilane coupling agents such as γ-aminophenyl-trimethoxysilane and N- (βaminoethyl) -γ-aminopropyltrimethoxysilane, vinyltriethoxysilane, vinyl-tris (2-methoxy-). Ethoxy) silane, γ-methacryloxypropyltrimethoxysilane and other cationic silane coupling agents, and β- (3,4-epoxycyclohexyl) ethyltrimethoxysilane, γ-glycidoxy-propyltrimethoxysilane and other epoxysilanes. System coupling agents and the like. Of these, when the thermosetting resin impregnated in the woven glass cloth is an epoxy resin, it is common to use a cationic silane coupling agent.
【０００４】[0004]
【発明が解決しようとする課題】しかし、低熱膨張のガ
ラス繊維で構成したガラス織布を使用する場合、ガラス
織布に含浸した樹脂とガラス繊維の界面での接着力が弱
く、プリント配線の基板として使用したときにマイグレ
ーションが発生しやすいという欠点があった。Ｅガラス
のガラス織布を使用した場合にはこのような問題は殊更
起こらず、れは低膨張ガラス繊維を含むガラス繊維で構
成したガラス織布を使用する場合に特有の問題である。
本発明が解決しようとする課題は、低熱膨張（熱膨張率
４ｐｐｍ／℃以下）のガラス繊維を含むガラス繊維で構
成したガラス織布を使用した積層板において、耐マイグ
レーション性を向上させることである。また、そのよう
な積層板を製造するためのプリプレグを製造することで
ある。さらには、前記積層板およびプリプレグを製造す
るためのガラス織布を提供することである。However, when a glass woven fabric composed of glass fibers having a low thermal expansion is used, the adhesive force at the interface between the resin impregnated in the glass woven fabric and the glass fibers is weak, and the printed wiring board However, there is a drawback that migration easily occurs when used as. Such a problem does not occur particularly when the glass woven cloth of E glass is used, and this is a problem specific to the case where the glass woven cloth composed of the glass fiber including the low expansion glass fiber is used.
The problem to be solved by the present invention is to improve migration resistance in a laminated sheet using a glass woven fabric composed of glass fibers containing glass fibers having a low thermal expansion (coefficient of thermal expansion of 4 ppm / ° C. or less). . Moreover, it is to manufacture a prepreg for manufacturing such a laminated board. Furthermore, it is providing the glass woven cloth for manufacturing the said laminated board and prepreg.
【０００５】[0005]
【課題を解決するための手段】上記課題を解決するため
に、本発明に係る積層板の製造法は、熱硬化性樹脂を含
浸したガラス織布を重ねて加熱加圧成形する方法におい
て、前記使用するガラス織布の一部ないし全部に、熱膨
張率４ｐｐｍ／℃以下のガラス繊維を含むガラス繊維で
構成したガラス織布を用いる。当該ガラス織布には、熱
硬化性樹脂の含浸に先立ち、下記に示す化学式（１）に
おいてｎが３以上であるシラン系カップリング剤で処理
をしておくことを特徴とする。In order to solve the above-mentioned problems, a method for manufacturing a laminated board according to the present invention is a method in which glass woven cloth impregnated with a thermosetting resin is layered and heated and pressure-molded. A glass woven cloth composed of glass fibers containing glass fibers having a coefficient of thermal expansion of 4 ppm / ° C. or less is used for a part or all of the glass woven cloth used. The glass woven fabric is characterized by being treated with a silane-based coupling agent having n of 3 or more in the chemical formula (1) shown below, prior to impregnation with the thermosetting resin.
【０００６】[0006]
【化４】 Embedded image
【０００７】（式中、Ｘは有機官能基 Ｙは加水分解性
基 ＲはＨ，ＣＨ3又はベンゼン環）シラン系カップリ
ング剤は、ガラス繊維表面に単分子膜を形成するような
量で適用される。Ｓガラス、Ｄガラス、Ｑガラスといっ
た熱膨張率が４ｐｐｍ／℃以下のガラス繊維を含むガラ
ス織布を用いた積層板においては、ガラス織布に含浸し
た樹脂とガラス繊維の熱膨張率の違いが大きいため、こ
れに起因して両者の界面に発生する応力も大きくなる。
本発明においては、化学式（１）においてｎを大きくす
ることによってカップリング剤の分子鎖を長くし、樹脂
とガラス繊維の界面に発生する応力を吸収して低減す
る。従って、積層板にドリル穴明け加工等の衝撃を加え
ても、微小クラックや、樹脂とガラス繊維の剥離を生じ
にくくなり、耐マイグレーション性に優れたスルーホー
ルの形成が可能となる。Ｅガラス繊維のように熱膨張率
の大きいガラス繊維で構成したガラス織布に対しては、
化学式（１）に示したシラン系カップリング剤を適用し
ても、殊更顕著な効果はなく、その効果は分子鎖の短い
シラン系カップリング剤を適用した場合と変わらない。
化学式（１）に示したシラン系カップリング剤は、熱膨
張率が４ｐｐｍ／℃以下のガラス繊維を含むガラス織布
と組み合わせて使用することにより、初めて顕著な効果
が現われる。(Wherein X is an organic functional group Y is a hydrolyzable group R is H, CH 3 or a benzene ring) The silane coupling agent is applied in an amount such that a monomolecular film is formed on the surface of the glass fiber. To be done. In a laminated plate using a glass woven cloth containing glass fibers having a thermal expansion coefficient of 4 ppm / ° C. or less such as S glass, D glass, and Q glass, the difference in the thermal expansion coefficient between the resin impregnated in the glass woven cloth and the glass fiber is Since it is large, the stress generated at the interface between the two is also large.
In the present invention, the molecular chain of the coupling agent is lengthened by increasing n in the chemical formula (1) to absorb and reduce the stress generated at the interface between the resin and the glass fiber. Therefore, even if an impact such as a drilling process is applied to the laminated plate, minute cracks and separation of the resin and the glass fiber are less likely to occur, and a through hole having excellent migration resistance can be formed. For a glass woven fabric composed of glass fibers having a large coefficient of thermal expansion such as E glass fibers,
Even if the silane coupling agent represented by the chemical formula (1) is applied, there is no particularly remarkable effect, and the effect is the same as when the silane coupling agent having a short molecular chain is applied.
The silane coupling agent represented by the chemical formula (1) exhibits a remarkable effect for the first time when it is used in combination with a glass woven fabric containing glass fibers having a thermal expansion coefficient of 4 ppm / ° C. or less.
【０００８】上記積層板の製造法において、ガラス織布
に含浸する熱硬化性樹脂として、フェノール樹脂を硬化
剤とするエポキシ樹脂を用いることができる。この場
合、化学式（１）に示したシラン系カップリング剤は、
有機官能基Ｘが好ましくはアミン系である。また、ガラ
ス織布に含浸する熱硬化性樹脂として、ジシアンジアミ
ドを硬化剤とするエポキシ樹脂を用いることができる。
この場合、化学式（１）に示したシラン系カップリング
剤は、有機官能基Ｘが好ましくはカチオニック系であ
る。In the above-mentioned method for producing a laminated plate, an epoxy resin containing a phenol resin as a curing agent can be used as the thermosetting resin impregnated in the glass woven cloth. In this case, the silane coupling agent represented by the chemical formula (1) is
The organic functional group X is preferably amine-based. As the thermosetting resin with which the woven glass cloth is impregnated, an epoxy resin using dicyandiamide as a curing agent can be used.
In this case, in the silane coupling agent represented by the chemical formula (1), the organic functional group X is preferably a cationic type.
【０００９】次に、本発明に係る積層板用プリプレグの
製造法は、ガラス織布に熱硬化性樹脂を含浸し乾燥する
方法において、前記ガラス織布として、熱膨張率４ｐｐ
ｍ／℃以下のガラス繊維を含むガラス繊維で構成したガ
ラス織布を用いる。当該ガラス織布には、熱硬化性樹脂
の含浸に先立ち、上記化学式（１）においてｎが３以上
であるシラン系カップリング剤で処理をしておくことを
特徴とする。含浸する熱硬化性樹脂とシラン系カップリ
ング剤の組み合わせは、上記積層板の製造法における熱
硬化性樹脂とシラン系カップリング剤の組み合わせと同
様の組み合わせが好ましい。Next, a method for manufacturing a prepreg for laminated plate according to the present invention is a method in which a glass woven cloth is impregnated with a thermosetting resin and dried, and the glass woven cloth has a coefficient of thermal expansion of 4 pp.
A glass woven fabric composed of glass fibers containing glass fibers of m / ° C. or less is used. The glass woven fabric is characterized in that it is treated with a silane coupling agent having n of 3 or more in the above chemical formula (1) prior to impregnation with the thermosetting resin. The combination of the thermosetting resin and the silane-based coupling agent to be impregnated is preferably the same as the combination of the thermosetting resin and the silane-based coupling agent in the method for producing a laminated plate.
【００１０】さらに、本発明に係る積層板用ガラス織布
は、熱膨張率４ｐｐｍ／℃以下のガラス繊維を含むガラ
ス繊維で構成したものであり、上記化学式（１）におい
てｎが３以上であるシラン系カップリング剤が付着して
いることを特徴とする。Further, the glass woven fabric for laminated plates according to the present invention is composed of glass fibers containing glass fibers having a coefficient of thermal expansion of 4 ppm / ° C. or less, and n in the above chemical formula (1) is 3 or more. It is characterized in that a silane coupling agent is attached.
【００１１】[0011]
【発明の実施の形態】本発明に係る積層板およびプリプ
レグに使用する樹脂は、その用途からエポキシ樹脂が一
般的であるがポリイミド、ＢＴ樹脂なども使用でき、特
に限定するものではない。使用するカップリング剤は、
エポキシ樹脂の場合、アミノシラン系やカチオニックシ
ラン系が望ましいが、化学式（１）の構造式を有するも
のであれば特にその種類を限定するものではない。本発
明に係るガラス織布は、種々の形態をとることができ
る。熱膨張率４ｐｐｍ／℃以下のガラス繊維のみで構成
したガラス織布をはじめとして、このようなガラス繊維
を一部に含むガラス織布であってもよい。例えば、ガラ
ス織布の縦糸又は横糸の一方だけに熱膨張率４ｐｐｍ／
℃以下のガラス繊維からなる糸を使用することができ
る。また、ガラス繊維を多数本収束して構成するガラス
糸自体の中に、熱膨張率４ｐｐｍ／℃以下のガラス繊維
を混在させることができる。このようなガラス織布のカ
ップリング剤による処理は、カップリング剤を溶媒に溶
かしてガラス織布に含浸させることで行なった。そのほ
か、ガラス繊維の段階やガラス繊維を収束したガラス糸
の段階で、カップリング剤による処理を行なってもよ
い。本発明に係る積層板は、熱硬化性樹脂を含浸乾燥し
たプリプレグを重ねて加熱加圧成形により製造する。こ
のとき、表面に銅箔等の金属箔を一体化してもよい。こ
の積層板にプリント配線を形成したプリント配線板を内
層や外層に配置した多層板も、本発明に係る積層板の概
念に含まれる。また、本発明に係る積層板用プリプレグ
は、積層板を製造するためのもののほか、プリント配線
板同士の間やプリント配線板と表面の金属箔の間に介在
させて、これらを加熱加圧成形により一体化して多層板
を製造するためのものも、その概念に含むものである。BEST MODE FOR CARRYING OUT THE INVENTION The resin used for the laminate and prepreg according to the present invention is generally an epoxy resin because of its use, but polyimide, BT resin, etc. can also be used, and there is no particular limitation. The coupling agent used is
In the case of the epoxy resin, an aminosilane type or a cationic silane type is desirable, but the type is not particularly limited as long as it has the structural formula of the chemical formula (1). The glass woven fabric according to the present invention can take various forms. A glass woven fabric composed only of glass fibers having a coefficient of thermal expansion of 4 ppm / ° C. or less, or a glass woven fabric partially containing such glass fibers may be used. For example, only one of warp or weft of glass woven fabric has a coefficient of thermal expansion of 4 ppm /
Threads composed of glass fibers below ℃ can be used. Further, glass fibers having a coefficient of thermal expansion of 4 ppm / ° C. or less can be mixed in the glass yarn itself which is formed by converging a large number of glass fibers. The treatment of such a glass woven cloth with the coupling agent was performed by dissolving the coupling agent in a solvent and impregnating the glass woven cloth. In addition, the treatment with the coupling agent may be performed at the stage of the glass fiber or the stage of the glass yarn in which the glass fibers are bundled. The laminated plate according to the present invention is manufactured by stacking prepregs impregnated with a thermosetting resin and drying them, and by heat-pressing. At this time, a metal foil such as a copper foil may be integrated on the surface. The multilayer board according to the present invention also includes a multilayer board in which a printed wiring board on which printed wiring is formed is arranged as an inner layer or an outer layer. Further, the prepreg for a laminated board according to the present invention is used not only for manufacturing a laminated board, but also between the printed wiring boards or between the printed wiring board and the metal foil on the surface, and heat and pressure molding them. The concept also includes a method for manufacturing a multilayer board by integrating the above.
【００１２】[0012]
【実施例】以下、本発明に係る実施例および参考例と従
来例を詳細に説明する。以下の実施例では、Ｓガラス組
成のガラス繊維で構成したガラス織布を使用している
が、熱膨張率４ｐｐｍ／℃以下のガラス繊維を含むガラ
ス繊維で構成したガラス織布を使用する限りは、表１に
示した実施例と同じ傾向の効果を得ることができる。EXAMPLES Examples, reference examples and conventional examples according to the present invention will be described in detail below. In the following examples, a glass woven fabric composed of glass fibers having an S glass composition is used, but as long as a glass woven fabric composed of glass fibers containing glass fibers having a thermal expansion coefficient of 4 ppm / ° C. or less is used. The effect of the same tendency as the embodiment shown in Table 1 can be obtained.
【００１３】（実施例１）Ｓガラス組成のガラス繊維
（熱膨張率：２．４ｐｐｍ／℃）で構成した厚み０．１
mm（ＭＩＬ規格＃２１１６）のガラス織布を準備した。
これを、化学式（２）に示すアミノシラン系カップリン
グ剤（γ−アミノブチル−トリメトキシシラン）で処理
した（ガラス織布ａ）。Example 1 A glass fiber having an S glass composition (coefficient of thermal expansion: 2.4 ppm / ° C.) having a thickness of 0.1
A glass woven fabric having a size of mm (MIL standard # 2116) was prepared.
This was treated with the aminosilane-based coupling agent (γ-aminobutyl-trimethoxysilane) represented by the chemical formula (2) (glass woven fabric a).
【００１４】[0014]
【化５】 Embedded image
【００１５】臭素化エピビス系エポキシ樹脂 ２００ｇ
（東都化成製「ＹＤＢ−５００ＥＫ８０」） エピビス系エポキシ樹脂 ４３ｇ（油化シェル製「Ｅｐ
−１００１ＥＫ７５」） クレゾールノボラック型エポキシ樹脂 １７０ｇ（東都
化成製「ＹＤＣＮ−７０４ＥＫ７５」） ノボラック型フェノール樹脂（硬化剤） １３０ｇ（大
日本インキ製「ＴＤ−２０９０ＥＫ６０」） ２−エチル４−メチルイミダゾール（触媒） ０．５ｇ を均一に溶かしフェノール樹脂硬化型エポキシ樹脂ワニ
スＡを調製した。ガラス織布ａにワニスＡを含浸、乾燥
して、樹脂含有量が４２重量％のプリプレグａを得た。
プリプレグａを８枚重ねた両側に厚さ１８μｍの電解銅
箔を重ね、これを熱媒油プレスにて温度２００℃、圧力
４０Kgf／cm2で９０分間加熱成形し、厚さ０．８mmの銅
張り積層板を得た。 （実施例２）Ｓガラス組成のガラス繊維（熱膨張率：
２．４ｐｐｍ／℃）で構成した厚み０．１mm（ＭＩＬ規
格＃２１１６）のガラス織布を準備した。これを、化学
式（３）示すアミノシラン系カップリング剤（γ−アミ
ノヘキシル−トリメトキシシラン）で処理した（ガラス
織布ｂ）。200 g of brominated epibis type epoxy resin
(Toto Kasei "YDB-500EK80") Epibis-based epoxy resin 43 g (Yuka Kagaku's "Ep"
-1001EK75 ") Cresol novolac type epoxy resin 170g (Toto Kasei" YDCN-704EK75 ") Novolac phenolic resin (curing agent) 130g (Dainippon Ink's" TD-2090EK60 ") 2-ethyl 4-methylimidazole (catalyst) A phenol resin-curable epoxy resin varnish A was prepared by uniformly dissolving 0.5 g. The glass woven fabric a was impregnated with the varnish A and dried to obtain a prepreg a having a resin content of 42% by weight.
Eight prepregs a were stacked on each other, 18 μm thick electrolytic copper foil was stacked on both sides, and this was heat-formed with a heat transfer oil press at a temperature of 200 ° C. and a pressure of 40 Kgf / cm 2 for 90 minutes to form a 0.8 mm thick copper foil. A tension laminate was obtained. (Example 2) Glass fiber of S glass composition (coefficient of thermal expansion:
A glass woven fabric having a thickness of 0.1 mm (MIL standard # 2116) composed of 2.4 ppm / ° C.) was prepared. This was treated with an aminosilane coupling agent (γ-aminohexyl-trimethoxysilane) represented by the chemical formula (3) (glass woven fabric b).
【００１６】[0016]
【化６】 [Chemical 6]
【００１７】ガラス織布ｂにワニスＡを含浸、乾燥し
て、樹脂含有量が４２重量％のプリプレグｂを得た。プ
リプレグｂを用いて実施例１と同様の工程で厚さ０．８
mmの銅張り積層板を得た。The glass woven fabric b was impregnated with the varnish A and dried to obtain a prepreg b having a resin content of 42% by weight. Using the prepreg b, the thickness is 0.8 in the same process as in the first embodiment.
A copper-clad laminate of mm was obtained.
【００１８】（実施例３）Ｓガラス組成のガラス繊維
（熱膨張率：２．４ｐｐｍ／℃）で構成した厚み０．１
mm（ＭＩＬ規格＃２１１６）のガラス織布を準備した。
これを、化学式（４）示すアミノシラン系カップリング
剤（γ−アミノイソペンチル−トリメトキシシラン）で
処理した（ガラス織布ｃ）。Example 3 A glass fiber having an S glass composition (coefficient of thermal expansion: 2.4 ppm / ° C.) having a thickness of 0.1
A glass woven fabric having a size of mm (MIL standard # 2116) was prepared.
This was treated with an aminosilane coupling agent (γ-aminoisopentyl-trimethoxysilane) represented by the chemical formula (4) (glass woven fabric c).
【００１９】[0019]
【化７】 [Chemical 7]
【００２０】ガラス織布ｃにワニスＡを含浸、乾燥し
て、樹脂含有量が４２重量％のプリプレグｃを得た。プ
リプレグｃを用いて実施例１と同様の工程で厚さ０．８
mmの銅張り積層板を得た。The woven glass cloth c was impregnated with the varnish A and dried to obtain a prepreg c having a resin content of 42% by weight. The thickness of the prepreg c is 0.8 in the same process as in Example 1.
A copper-clad laminate of mm was obtained.
【００２１】（実施例４）Ｓガラス組成のガラス繊維
（熱膨張率：２．４ｐｐｍ／℃）で構成した厚み０．１
mm（ＭＩＬ規格＃２１１６）のガラス織布を準備した。
これを、化学式（５）に示すカチオニック系シランカッ
プリング剤（γ−メタクリロキシブチル−トリメトキシ
シラン）で処理した（ガラス織布ｄ）。Example 4 A glass fiber having an S glass composition (coefficient of thermal expansion: 2.4 ppm / ° C.) having a thickness of 0.1
A glass woven fabric having a size of mm (MIL standard # 2116) was prepared.
This was treated with a cationic silane coupling agent (γ-methacryloxybutyl-trimethoxysilane) represented by the chemical formula (5) (glass woven fabric d).
【００２２】[0022]
【化８】 Embedded image
【００２３】臭素化エピビス系エポキシ樹脂 ２００ｇ
（東都化成製 ＹＤＢ−５００ＥＫ８０） エピビス系エポキシ樹脂 １２８ｇ（油化シェル製 Ｅ
ｐ−１００１ＥＫ７５） クレゾールノボラック型エポキシ樹脂 ８５ｇ（東都化
成製 ＹＤＣＮ−７０４ＥＫ７５） ジシアンジアミド（ＤＩＣＹ，硬化剤） ９ｇ（メチル
グリコール１００ｇに溶解） ２−エチル４−メチルイミダゾール（触媒） ０．６ｇ を均一に溶かしジシアンジアミド硬化型エポキシ樹脂ワ
ニスＢを調製した。ガラス織布ｄにワニスＢを含浸、乾
燥して、樹脂含有量が４２重量％のプリプレグｄを得
た。プリプレグｄを用いて実施例１と同様の工程で厚さ
０．８mmの銅張り積層板を得た。200 g of brominated epibis type epoxy resin
(YDB-500EK80 manufactured by Tohto Kasei) 128 g of epibis-based epoxy resin (E manufactured by Yuka Shell
p-1001EK75) Cresol novolac type epoxy resin 85 g (Toto Kasei YDCN-704EK75) Dicyandiamide (DICY, curing agent) 9 g (dissolved in methyl glycol 100 g) 2-Ethyl 4-methylimidazole (catalyst) 0.6 g was uniformly dissolved. A dicyandiamide curable epoxy resin varnish B was prepared. The glass woven fabric d was impregnated with the varnish B and dried to obtain a prepreg d having a resin content of 42% by weight. A copper-clad laminate having a thickness of 0.8 mm was obtained in the same process as in Example 1 using the prepreg d.
【００２４】（実施例５）Ｓガラス組成のガラス繊維
（熱膨張率：２．４ｐｐｍ／℃）で構成した厚み０．１
mm（ＭＩＬ規格＃２１１６）のガラス織布を準備した。
これを、化学式（６）に示すカチオニック系シランカッ
プリング剤（γ−メタクリロキシヘキシル−トリメトキ
シシラン）で処理した（ガラス織布ｅ）。Example 5 A glass fiber having an S glass composition (coefficient of thermal expansion: 2.4 ppm / ° C.) having a thickness of 0.1
A glass woven fabric having a size of mm (MIL standard # 2116) was prepared.
This was treated with a cationic silane coupling agent (γ-methacryloxyhexyl-trimethoxysilane) represented by the chemical formula (6) (glass woven fabric e).
【００２５】[0025]
【化９】 Embedded image
【００２６】ガラス織布ｅにワニスＢを含浸、乾燥し
て、樹脂含有量が４２重量％のプリプレグｅを得た。プ
リプレグｅを用いて実施例１と同様の工程で厚さ０．８
mmの銅張り積層板を得た。Glass woven fabric e was impregnated with varnish B and dried to obtain prepreg e having a resin content of 42% by weight. Using the prepreg e, the thickness is 0.8 in the same process as in Example 1.
A copper-clad laminate of mm was obtained.
【００２７】（実施例６）Ｓガラス組成のガラス繊維
（熱膨張率：２．４ｐｐｍ／℃）で構成した厚み０．１
mm（ＭＩＬ規格＃２１１６）のガラス織布を準備した。
これを、化学式（７）に示すカチオニック系シランカッ
プリング剤（γ−メタクリロキシイソペンチル−トリメ
トキシシラン）で処理した（ガラス織布ｆ）。Example 6 A glass fiber having an S glass composition (coefficient of thermal expansion: 2.4 ppm / ° C.) having a thickness of 0.1
A glass woven fabric having a size of mm (MIL standard # 2116) was prepared.
This was treated with a cationic silane coupling agent (γ-methacryloxyisopentyl-trimethoxysilane) represented by the chemical formula (7) (glass woven fabric f).
【００２８】[0028]
【化１０】 Embedded image
【００２９】ガラス織布ｆにワニスＢを含浸、乾燥さ
せ、樹脂含有量が４２重量％のプリプレグｆを得た。プ
リプレグｆを用いて実施例１と同様の工程で厚さ０．８
mmの銅張り積層板を得た。The glass woven fabric f was impregnated with the varnish B and dried to obtain a prepreg f having a resin content of 42% by weight. Using the prepreg f, the thickness is 0.8 in the same process as in the first embodiment.
A copper-clad laminate of mm was obtained.
【００３０】（実施例７）ガラス織布ｂにワニスＢを含
浸、乾燥して、樹脂含有量が４２重量％のプリプレグｇ
を得た。プリプレグｇを用いて実施例１と同様の工程で
厚さ０．８mmの銅張り積層板を得た。Example 7 A glass woven fabric b was impregnated with varnish B and dried to obtain a prepreg g having a resin content of 42% by weight.
I got A copper-clad laminate having a thickness of 0.8 mm was obtained by the same process as in Example 1 using the prepreg g.
【００３１】（実施例８）ガラス織布ｅにワニスＡを含
浸、乾燥して、樹脂含有量が４２重量％のプリプレグｈ
を得た。プリプレグｈを用いて実施例１と同様の工程で
厚さ０．８mmの銅張り積層板を得た。(Embodiment 8) Glass woven fabric e is impregnated with varnish A and dried to prepare a prepreg h having a resin content of 42% by weight.
I got Using the prepreg h, a copper-clad laminate having a thickness of 0.8 mm was obtained in the same process as in Example 1.
【００３２】（従来例１）Ｓガラス組成のガラス繊維
（熱膨張率：２．４ｐｐｍ／℃）で構成した厚み０．１
mm（ＭＩＬ規格＃２１１６）のガラス織布を準備した。
これを、化学式（８）に示すアミノシラン系カップリン
グ剤（γ−アミノプロピル−トリメトキシシラン）で処
理した（ガラス織布ｇ）。(Conventional Example 1) Thickness 0.1 composed of glass fibers of S glass composition (coefficient of thermal expansion: 2.4 ppm / ° C.)
A glass woven fabric having a size of mm (MIL standard # 2116) was prepared.
This was treated with an aminosilane coupling agent (γ-aminopropyl-trimethoxysilane) represented by the chemical formula (8) (glass woven fabric g).
【００３３】[0033]
【化１１】 Embedded image
【００３４】ガラス織布ｇにワニスＡを含浸、乾燥さ
せ、樹脂含有量が４２重量％のプリプレグｉを得た。プ
リプレグｉを用いて実施例１と同様の工程で厚さ０．８
mmの銅張り積層板を得た。Glass woven fabric g was impregnated with varnish A and dried to obtain a prepreg i having a resin content of 42% by weight. The thickness of the prepreg i is 0.8 in the same process as in the first embodiment.
A copper-clad laminate of mm was obtained.
【００３５】（従来例２）Ｓガラス組成のガラス繊維
（熱膨張率：２．４ｐｐｍ／℃）で構成した厚み０．１
mm（ＭＩＬ規格＃２１１６）のガラス織布を準備した。
これを、化学式（９）に示すカチオニックシラン系カッ
プリング剤（γ−メタクリロキシプロピル−トリメトキ
シシラン）で処理した（ガラス織布ｈ）。(Conventional Example 2) A thickness of 0.1 composed of glass fibers of S glass composition (coefficient of thermal expansion: 2.4 ppm / ° C.)
A glass woven fabric having a size of mm (MIL standard # 2116) was prepared.
This was treated with a cationic silane coupling agent (γ-methacryloxypropyl-trimethoxysilane) represented by the chemical formula (9) (glass woven fabric h).
【００３６】[0036]
【化１２】 [Chemical 12]
【００３７】ガラス織布ｈにワニスＢを含浸、乾燥さ
せ、樹脂含有量が４２重量％のプリプレグｊを得た。プ
リプレグｊを用いて実施例１と同様の工程で厚さ０．８
mmの銅張り積層板を得た。The glass woven fabric h was impregnated with the varnish B and dried to obtain a prepreg j having a resin content of 42% by weight. The thickness of the prepreg j is 0.8 in the same process as in the first embodiment.
A copper-clad laminate of mm was obtained.
【００３８】（参考例１）Ｅガラス組成のガラス繊維
（熱膨張率：５．６ｐｐｍ／℃）で構成した厚み０．１
mm（ＭＩＬ規格＃２１１６）のガラス織布を準備した。
これを、実施例２で使用したアミノシラン系カップリン
グ剤（γ−アミノヘキシル−トリメトキシシラン）で処
理した（ガラス織布ｉ）。ガラス織布ｉにワニスＡを含
浸、乾燥し、樹脂含有量が４２重量％のプリプレグｋを
得た。プリプレグｋを用いて実施例１と同様の工程で厚
さ０．８mmの銅張り積層板を得た。Reference Example 1 A glass fiber of E glass composition (coefficient of thermal expansion: 5.6 ppm / ° C.) having a thickness of 0.1
A glass woven fabric having a size of mm (MIL standard # 2116) was prepared.
This was treated with the aminosilane coupling agent (γ-aminohexyl-trimethoxysilane) used in Example 2 (glass woven fabric i). The glass woven fabric i was impregnated with the varnish A and dried to obtain a prepreg k having a resin content of 42% by weight. A copper-clad laminate having a thickness of 0.8 mm was obtained in the same process as in Example 1 using the prepreg k.
【００３９】（参考例２）Ｅガラス組成のガラス繊維
（熱膨張率：５．６ｐｐｍ／℃）で構成した厚み０．１
mm（ＭＩＬ規格＃２１１６）のガラス織布を準備した。
これを、参考例１で使用したアミノシラン系カップリン
グ剤（γ−アミノプロピル−トリメトキシシラン）で処
理した（ガラス織布ｊ）。ガラス織布ｊにワニスＡを含
浸、乾燥し、樹脂含有量が４２重量％のプリプレグｌを
得た。プリプレグｌを用いて実施例１と同様の工程で厚
さ０．８mmの銅張り積層板を得た。Reference Example 2 A glass fiber having an E glass composition (coefficient of thermal expansion: 5.6 ppm / ° C.) having a thickness of 0.1
A glass woven fabric having a size of mm (MIL standard # 2116) was prepared.
This was treated with the aminosilane coupling agent (γ-aminopropyl-trimethoxysilane) used in Reference Example 1 (glass woven fabric j). The glass woven fabric j was impregnated with the varnish A and dried to obtain a prepreg 1 having a resin content of 42% by weight. A copper-clad laminate having a thickness of 0.8 mm was obtained by the same process as in Example 1 using the prepreg 1.
【００４０】実施例１〜８、従来例１〜２、参考例１〜
２における銅張り積層板の特性を表１に示す。表中、耐
マイグレーション性は以下のようにして評価した。図１
に示すような回路パターンに銅張り積層板を回路加工
し、相対する１００個のスルーホールを形成したサンプ
ル（１５個）を用意する。スルーホール２は、穴径０．
４mm，穴壁間隔０．３mm，スルーホールメッキ厚２５μ
ｍである。ランド１の径は、０．４mmである。図中、回
路の点線は、裏面側の回路を示す。これに、８５℃／８
５％ＲＨの雰囲気で直流５０Ｖの電圧を１００時間かけ
続けた後のショート発生サンプル数を数えた。Examples 1-8, Conventional Examples 1-2, Reference Examples 1-
Table 1 shows the characteristics of the copper-clad laminate in No. 2. In the table, the migration resistance was evaluated as follows. FIG.
Samples (15 pieces) in which a copper-clad laminate is processed into a circuit pattern as shown in (5) to form 100 through holes facing each other are prepared. The through hole 2 has a hole diameter of 0.
4mm, hole wall spacing 0.3mm, through hole plating thickness 25μ
m. The diameter of the land 1 is 0.4 mm. In the figure, the dotted line of the circuit shows the circuit on the back side. To this, 85 ℃ / 8
The number of short-circuited samples was counted after continuously applying a DC voltage of 50 V for 100 hours in an atmosphere of 5% RH.
【００４１】[0041]
【表１】 [Table 1]
【００４２】[0042]
【発明の効果】本発明においては、熱膨張率が４ｐｐｍ
／℃以下のガラス繊維を含むガラス織布を使用した積層
板の製造において、前記ガラス織布に化学式（１）に示
す構造式のシラン系カップリング剤のｎが３以上である
ものを組み合わせることにより、ガラス繊維と樹脂の熱
膨張率の差に起因して両者の界面に発生するよる応力を
吸収することができる。前記応力が小さい状態で、積層
板のドリル穴明けをすることができるので、ドリル穴明
け時の衝撃による微少クラック等を防ぐことができる
（前記応力が存在した状態にあると、その応力を解放し
ようとして小さな衝撃によってもクラックが入りやす
い）。その結果、耐マイグレーション性に優れた低熱膨
張の積層板を得ることができる。ガラス織布に含浸する
熱硬化性樹脂として、フェノール樹脂を硬化剤とするエ
ポキシ樹脂を用いる場合、化学式（１）に示したシラン
系カップリング剤として有機官能基Ｘがアミン系のもの
を用いると、上記効果は一層顕著になる。また、ジシア
ンジアミドを硬化剤とするエポキシ樹脂を用いる場合、
化学式（１）に示したシラン系カップリング剤として有
機官能基Ｘがカチオニック系のものを用いると、同様に
上記効果は一層顕著になる。これらの場合において、化
学式（１）におけるｎの数が４以上であるとさらに好ま
しい結果が得られる。According to the present invention, the coefficient of thermal expansion is 4 ppm.
In the production of a laminated sheet using a glass woven fabric containing glass fibers at a temperature of / ° C or lower, combining the glass woven fabric with a silane coupling agent having a structural formula represented by the chemical formula (1) in which n is 3 or more. This makes it possible to absorb the stress generated at the interface between the glass fiber and the resin due to the difference in coefficient of thermal expansion between them. Since the drilling of the laminated plate can be done in the state where the stress is small, it is possible to prevent minute cracks etc. due to the impact at the time of drilling (when the stress exists, the stress is released. Even if you try to make a small impact, cracks easily occur). As a result, it is possible to obtain a laminate having low thermal expansion and excellent migration resistance. When an epoxy resin using a phenol resin as a curing agent is used as the thermosetting resin impregnated in the glass woven cloth, if the organic functional group X is an amine-based one as the silane coupling agent represented by the chemical formula (1). The above effect becomes more remarkable. When an epoxy resin containing dicyandiamide as a curing agent is used,
If the organic functional group X having a cationic group is used as the silane coupling agent represented by the chemical formula (1), the above effect becomes more remarkable. In these cases, more preferable results are obtained when the number of n in the chemical formula (1) is 4 or more.
【図１】積層板の耐マイグレーション性を評価するため
に使用した回路パターンの説明図である。FIG. 1 is an explanatory diagram of a circuit pattern used to evaluate migration resistance of a laminated board.
Claims (8)
て加熱加圧成形する積層板の製造において、 前記ガラス織布の一部ないし全部が、熱膨張率４ｐｐｍ
／℃以下のガラス繊維を含むガラス繊維で構成したガラ
ス織布であり、 熱硬化性樹脂の含浸に先立ち、当該ガラス織布を下記に
示す化学式（１）においてｎが３以上であるシラン系カ
ップリング剤で処理することを特徴とする積層板の製造
法。 【化１】 （式中、Ｘは有機官能基 Ｙは加水分解性基 ＲはＨ，
ＣＨ3又はベンゼン環）1. In the production of a laminated sheet in which glass woven fabrics impregnated with a thermosetting resin are stacked and heat-pressed, a part or all of the glass woven fabrics has a coefficient of thermal expansion of 4 ppm.
A glass woven fabric composed of glass fibers containing a glass fiber having a temperature of / ° C or lower, and prior to impregnation with a thermosetting resin, the glass woven fabric is a silane-based cup in which n is 3 or more in the chemical formula (1) shown below. A method for producing a laminate, which comprises treating with a ring agent. Embedded image (In the formula, X is an organic functional group, Y is a hydrolyzable group, R is H,
CH 3 or benzene ring)
するエポキシ樹脂である請求項１項記載の積層板の製造
法。2. The method for producing a laminated board according to claim 1, wherein the thermosetting resin is an epoxy resin containing a phenol resin as a curing agent.
グ剤の有機官能基Ｘがアミン系である請求項２項記載の
積層板の製造法。3. The method for producing a laminated sheet according to claim 2, wherein the organic functional group X of the silane coupling agent in the chemical formula (1) is amine.
とするエポキシ樹脂である請求項１項記載の積層板の製
造法。4. The method for producing a laminated board according to claim 1, wherein the thermosetting resin is an epoxy resin containing dicyandiamide as a curing agent.
グ剤の有機官能基Ｘがカチオニック系である請求項４項
記載の積層板の製造法。5. The method for producing a laminated sheet according to claim 4, wherein the organic functional group X of the silane coupling agent in the chemical formula (1) is a cationic group.
グ剤のｎが４以上である請求項３又は５に記載の積層板
の製造法。6. The method for producing a laminated sheet according to claim 3, wherein n of the silane coupling agent in the chemical formula (1) is 4 or more.
る積層板用プリプレグの製造において、 前記ガラス織布が、熱膨張率４ｐｐｍ／℃以下のガラス
繊維を含むガラス繊維で構成したガラス織布であり、 熱硬化性樹脂の含浸に先立ち、当該ガラス織布を下記に
示す化学式（１）においてｎが３以上であるシラン系カ
ップリング剤で処理することを特徴とする積層板用プリ
プレグの製造法。 【化２】 （式中、Ｘは有機官能基 Ｙは加水分解性基 ＲはＨ，
ＣＨ3又はベンゼン環）7. A prepreg for a laminated plate, which is obtained by impregnating a glass woven cloth with a thermosetting resin and drying the glass, wherein the glass woven cloth is composed of glass fibers containing glass fibers having a coefficient of thermal expansion of 4 ppm / ° C. or less. A prepreg for a laminated plate, which is a woven fabric, wherein the glass woven fabric is treated with a silane coupling agent in which n is 3 or more in the chemical formula (1) shown below, prior to impregnation with a thermosetting resin. Manufacturing method. Embedded image (In the formula, X is an organic functional group, Y is a hydrolyzable group, R is H,
CH 3 or benzene ring)
含むガラス繊維で構成したガラス織布であり、 ガラス繊維に下記に示す化学式（１）においてｎが３以
上であるシラン系カップリング剤が付着していることを
特徴とする積層板用ガラス織布。 【化３】 （式中、Ｘは有機官能基 Ｙは加水分解性基 ＲはＨ，
ＣＨ3又はベンゼン環）8. A woven woven cloth composed of glass fibers containing glass fibers having a coefficient of thermal expansion of 4 ppm / ° C. or less, wherein the glass fibers are silane coupling agents in which n is 3 or more in the chemical formula (1) shown below. A glass woven fabric for laminated plates, which is characterized by having adhered thereto. Embedded image (In the formula, X is an organic functional group, Y is a hydrolyzable group, R is H,
CH 3 or benzene ring)
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP24604995A JPH0985891A (en) | 1995-09-25 | 1995-09-25 | Manufacture of laminated board, manufacture of prepreg for the laminated board and glass woven fabric for the laminated board |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP24604995A JPH0985891A (en) | 1995-09-25 | 1995-09-25 | Manufacture of laminated board, manufacture of prepreg for the laminated board and glass woven fabric for the laminated board |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH0985891A true JPH0985891A (en) | 1997-03-31 |
Family
ID=17142712
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP24604995A Pending JPH0985891A (en) | 1995-09-25 | 1995-09-25 | Manufacture of laminated board, manufacture of prepreg for the laminated board and glass woven fabric for the laminated board |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH0985891A (en) |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2009070921A (en) * | 2007-09-11 | 2009-04-02 | Sumitomo Bakelite Co Ltd | Insulative resin sheet containing glass woven fabric, laminate sheet, multilayer printed wiring board, and semiconductor device |
| JP2011216892A (en) * | 2011-05-16 | 2011-10-27 | Sumitomo Bakelite Co Ltd | Insulative resin sheet containing glass woven fabric, laminate plate, multilayer printed wiring board, and semiconductor device |
-
1995
- 1995-09-25 JP JP24604995A patent/JPH0985891A/en active Pending
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2009070921A (en) * | 2007-09-11 | 2009-04-02 | Sumitomo Bakelite Co Ltd | Insulative resin sheet containing glass woven fabric, laminate sheet, multilayer printed wiring board, and semiconductor device |
| JP2011216892A (en) * | 2011-05-16 | 2011-10-27 | Sumitomo Bakelite Co Ltd | Insulative resin sheet containing glass woven fabric, laminate plate, multilayer printed wiring board, and semiconductor device |
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