JP3322123B2 - Prepreg and laminate using the same - Google Patents
Prepreg and laminate using the sameInfo
- Publication number
- JP3322123B2 JP3322123B2 JP10673496A JP10673496A JP3322123B2 JP 3322123 B2 JP3322123 B2 JP 3322123B2 JP 10673496 A JP10673496 A JP 10673496A JP 10673496 A JP10673496 A JP 10673496A JP 3322123 B2 JP3322123 B2 JP 3322123B2
- Authority
- JP
- Japan
- Prior art keywords
- resin composition
- weight
- thermosetting resin
- prepreg
- parts
- 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 - Fee Related
Links
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- Reinforced Plastic Materials (AREA)
- Moulding By Coating Moulds (AREA)
- Compositions Of Macromolecular Compounds (AREA)
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、電気・電子機器等
に使用されるプリント配線板の製造に用いられるプリプ
レグ及び積層板に関するものである。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a prepreg and a laminate used for manufacturing a printed wiring board used for electric / electronic equipment and the like.
【０００２】[0002]
【従来の技術】従来、プリント配線板の製造に用いられ
る積層板は、例えばガラスクロス等の基材にエポキシ樹
脂等の熱硬化性樹脂組成物を含浸した後、乾燥して半硬
化させることによってプリプレグを作製し、このプリプ
レグを所要枚数重ねるとともに、必要に応じて銅箔等の
金属箔をその片側又は両側に配して積層した後、加熱加
圧をすることにより成形を行って製造されている。2. Description of the Related Art Conventionally, a laminated board used for manufacturing a printed wiring board is obtained by impregnating a base material such as a glass cloth with a thermosetting resin composition such as an epoxy resin, and then drying and semi-curing. A prepreg is manufactured, and a required number of prepregs are stacked, and if necessary, a metal foil such as a copper foil is laminated on one or both sides thereof, and then molded by heating and pressing. I have.
【０００３】近年のプリント配線板の高密度実装化等の
進行に伴い、積層板の低誘電率化や軽量化等の諸特性の
改良が求められている。その対応として、ガラスクロス
に代えて、アラミドクロスや、アラミドペーパーを基材
として用いた積層板が提案されている（例えば特開平１
−１１８５３９号）。[0003] With the progress of high-density mounting of printed wiring boards in recent years, there has been a demand for improvements in various characteristics such as lowering of the dielectric constant and weight reduction of laminated boards. As a countermeasure, an aramid cloth or a laminated board using aramid paper as a base material has been proposed instead of a glass cloth (for example, Japanese Patent Laid-Open No.
-118539).
【０００４】このアラミドペーパーはアラミド繊維を必
要に応じてバインダーとともに抄紙した後、温度及び圧
力をかけて製造したり、同様にして抄紙したものを複数
枚重ね、温度及び圧力をかけて１枚化して製造されてい
る。[0004] This aramid paper is made by making aramid fibers together with a binder, if necessary, and then by applying temperature and pressure, or by stacking a plurality of sheets made in the same manner and by applying temperature and pressure to make one sheet. Manufactured.
【０００５】しかし、一般にアラミド繊維は、短繊維に
するのが難しいため、抄紙するときの繊維の分散性が悪
く、アラミドペーパーは繊維密度の面内ばらつきが大き
いのが現状である。そのため、アラミドペーパーを基材
として用いて熱硬化性樹脂組成物を含浸して製造するプ
リプレグは、アラミドペーパーの繊維密度のばらつきの
影響により、表面平滑性が劣るという問題があった。こ
の表面平滑性が劣るプリプレグを用いて成形して得られ
た積層板は、積層板中に気泡が残留し、その積層板を用
いてプリント配線板を製造すると、その気泡にメッキ液
が浸入して絶縁不良を起こし、電気的信頼性を低下させ
る場合があるという問題があり、表面平滑性が優れたプ
リプレグが求められている。However, since aramid fibers are generally difficult to be made into short fibers, the dispersibility of the fibers during papermaking is poor, and at present the aramid paper has large in-plane variations in fiber density. Therefore, a prepreg manufactured by impregnating a thermosetting resin composition using aramid paper as a base material has a problem that surface smoothness is poor due to the influence of variation in fiber density of aramid paper. In a laminate obtained by molding using a prepreg having poor surface smoothness, bubbles remain in the laminate, and when a printed wiring board is manufactured using the laminate, a plating solution enters the bubbles. Therefore, there is a problem that insulation failure may occur and electrical reliability may be reduced, and a prepreg having excellent surface smoothness is required.
【０００６】[0006]
【発明が解決しようとする課題】本発明は、上記問題点
を改善するために成されたもので、その目的とするとこ
ろは、熱硬化性樹脂組成物をアラミドペーパーに含浸し
てなるプリプレグであって、表面平滑性が優れたプリプ
レグを提供することにある。またこのプリプレグを用い
て製造した気泡の残留が少ない積層板を提供することに
ある。SUMMARY OF THE INVENTION The present invention has been made to solve the above problems, and an object of the present invention is to provide a prepreg obtained by impregnating a thermosetting resin composition into aramid paper. It is another object of the present invention to provide a prepreg having excellent surface smoothness. Another object of the present invention is to provide a laminated board produced by using the prepreg and having less residual air bubbles.
【０００７】[0007]
【課題を解決するための手段】本発明の請求項１記載の
プリプレグは、熱硬化性樹脂組成物固形分１００重量部
に対し、平均粒子径が１〜１０μｍの無機充填材であっ
て、ガラスの粉末又はタルクの粉末である無機充填材を
１〜１０重量部含有する熱硬化性樹脂組成物を、ポリパ
ラフェニレンテレフタルアミドであるアラミドの繊維を
抄紙して製造しているアラミドペーパーに含浸してなる
ことを特徴とする。The prepreg of claim 1 wherein the SUMMARY OF THE INVENTION The present invention is, with respect to the thermosetting resin composition 100 parts by weight of the solid content, average particle diameter encounters 1~10μm inorganic filler
A thermosetting resin composition containing 1 to 10 parts by weight of an inorganic filler which is a powder of glass or a powder of talc ;
Aramid fiber which is raphenylene terephthalamide
It is characterized by being impregnated into aramid paper manufactured by papermaking .
【０００８】本発明の請求項２記載のプリプレグは、請
求項１記載のプリプレグにおいて、無機充填材が、Ｅガ
ラスの粉末を含有することを特徴とする。A prepreg according to a second aspect of the present invention is the prepreg according to the first aspect, wherein the inorganic filler contains E glass powder.
【０００９】本発明の請求項３記載のプリプレグは、請
求項１又は請求項２記載のプリプレグにおいて、熱硬化
性樹脂組成物が、エポキシ樹脂系樹脂組成物であること
を特徴とする。A prepreg according to a third aspect of the present invention is the prepreg according to the first or second aspect, wherein the thermosetting resin composition is an epoxy resin-based resin composition.
【００１０】本発明の請求項４記載の積層板は、請求項
１から請求項３のいずれかに記載のプリプレグを用いて
成形してなることを特徴とする。A laminate according to a fourth aspect of the present invention is characterized by being formed using the prepreg according to any one of the first to third aspects.
【００１１】本発明によると、熱硬化性樹脂組成物中に
適度な無機充填材を含有するため、含有しない場合と比
較して見かけの粘度がやや大きくなり、熱硬化性樹脂組
成物がアラミドペーパーの低密度の部分に多く保持され
ることにより表面平滑性が優れたプリプレグとなると考
えられる。また、この表面平滑性が優れたプリプレグを
用いるため、プリプレグとプリプレグや、プリプレグと
金属箔等を積層したときその間に抱き込む空気の量が少
なくなり、成形すると気泡の残留が少ない積層板とな
る。According to the present invention, since the thermosetting resin composition contains a suitable inorganic filler, the apparent viscosity is slightly larger than that when the thermosetting resin composition is not contained. It is considered that a prepreg having excellent surface smoothness is obtained by being retained in a low density portion of the prepreg. In addition, since this prepreg having excellent surface smoothness is used, when prepreg and prepreg, or prepreg and metal foil, etc. are laminated, the amount of air embraced therebetween is reduced, and when molded, a laminated plate with less air bubbles remains. .
【００１２】[0012]
【発明の実施の形態】本発明の請求項１から請求項３に
係るプリプレグは、熱硬化性樹脂組成物固形分１００重
量部に対し、平均粒子径が１〜１０μｍの無機充填材を
１〜１０重量部含有する熱硬化性樹脂組成物をアラミド
ペーパーに含浸したものであり、その熱硬化性樹脂組成
物としては、例えば、エポキシ樹脂系、フェノール樹脂
系、ポリイミド樹脂系、不飽和ポリエステル樹脂系、ポ
リフェニレンエーテル樹脂系等の単独、変性物、混合物
のように、熱硬化性樹脂組成物全般が挙げられる。な
お、この熱硬化性樹脂組成物は、アラミドペーパーに含
浸された後、必要に応じて加熱乾燥されていてもよい。BEST MODE FOR CARRYING OUT THE INVENTION The prepreg according to any one of claims 1 to 3 of the present invention comprises an inorganic filler having an average particle diameter of 1 to 10 μm per 100 parts by weight of a solid content of a thermosetting resin composition. Aramid paper is impregnated with a thermosetting resin composition containing 10 parts by weight. Examples of the thermosetting resin composition include epoxy resin, phenol resin, polyimide resin, and unsaturated polyester resin. And thermosetting resin compositions, such as polyphenylene ether resin alone, modified products, and mixtures. In addition, after this thermosetting resin composition is impregnated in aramid paper, it may be heated and dried as necessary.
【００１３】この熱硬化性樹脂組成物中には、熱硬化性
樹脂及び無機充填材を必須として含有し、必要に応じて
その熱硬化性樹脂の硬化剤、硬化促進剤、溶剤等を含有
することができる。なおエポキシ樹脂等のように自己硬
化性の低い熱硬化性樹脂は、その樹脂を硬化するための
硬化剤等も含有することが必要である。The thermosetting resin composition contains a thermosetting resin and an inorganic filler as essential components and, if necessary, a curing agent, a curing accelerator, a solvent and the like for the thermosetting resin. be able to. Note that a thermosetting resin having a low self-curing property, such as an epoxy resin, must also contain a curing agent for curing the resin.
【００１４】なお、熱硬化性樹脂組成物が、エポキシ樹
脂系の場合、電気特性及び接着性のバランスが良好であ
り好ましい。また、ポリイミド樹脂系の場合、誘電率が
低く好ましい。エポキシ樹脂系の樹脂組成物に含有する
エポキシ樹脂としては、例えばビスフェノールＡ型エポ
キシ樹脂、ビスフェノールＦ型エポキシ樹脂、ビスフェ
ノールＳ型エポキシ樹脂、フェノールノボラック型エポ
キシ樹脂、ビスフェノールＡノボラック型エポキシ樹
脂、ビスフェノールＦノボラック型エポキシ樹脂、クレ
ゾールノボラック型エポキシ樹脂、ジアミノジフェニル
メタン型エポキシ樹脂、及びこれらのエポキシ樹脂構造
体中の水素原子の一部をハロゲン化することにより難燃
化したエポキシ樹脂等が挙げられる。また、このエポキ
シ樹脂系の樹脂組成物に含有する硬化剤としては、例え
ばジシアンジアミド、脂肪族ポリアミド等のアミド系硬
化剤や、アンモニア、トリエチルアミン、ジエチルアミ
ン等のアミン系硬化剤や、フェノールノボラック樹脂、
クレゾールノボラック樹脂、ｐ−キシレン−ノボラック
樹脂等のフェノール系硬化剤や、酸無水物類等が挙げら
れる。なお、フェノール系硬化剤を用いると、この樹脂
組成物の硬化物の誘電特性が優れ好ましい。[0014] When the thermosetting resin composition is an epoxy resin-based composition, the electrical properties and the adhesiveness are well balanced, which is preferable. In the case of a polyimide resin, the dielectric constant is preferably low. Examples of the epoxy resin contained in the epoxy resin-based resin composition include bisphenol A epoxy resin, bisphenol F epoxy resin, bisphenol S epoxy resin, phenol novolak epoxy resin, bisphenol A novolak epoxy resin, and bisphenol F novolak. Type epoxy resin, cresol novolak type epoxy resin, diaminodiphenylmethane type epoxy resin, and an epoxy resin flame-retarded by halogenating a part of hydrogen atoms in these epoxy resin structures. As the curing agent contained in the epoxy resin-based resin composition, for example, amide-based curing agent such as dicyandiamide, aliphatic polyamide, ammonia, triethylamine, amine-based curing agent such as diethylamine, phenol novolak resin,
Examples include phenolic curing agents such as cresol novolak resin and p-xylene-novolak resin, and acid anhydrides. When a phenolic curing agent is used, the cured product of this resin composition has excellent dielectric properties, and is thus preferable.
【００１５】なお、この熱硬化性樹脂組成物の固形分１
００重量部中に、平均粒子径が１〜１０μｍの無機充填
材を１〜１０重量部含有することが重要である。平均粒
子径が１０μｍを超える場合は、熱硬化性樹脂組成物中
で無機充填材が沈降しやすく、無機充填材の濃度差が発
生しやすいため、アラミドペーパー表面に付着する無機
充填材の付着量にばらつきが発生して表面平滑性を改良
する効果が均一には得られにくく、平均粒子径が１μｍ
未満の場合は熱硬化性樹脂組成物中での無機充填材の分
散性が悪いため、均一に分散させようとすると混合のた
めの撹拌時間が長くなったり、撹拌条件を激しくする必
要があり実用的でない。また、無機充填材の比率が１重
量部未満の場合は、表面平滑性を改良する効果が小さ
く、１０重量部を越える場合は、熱硬化性樹脂組成物の
アラミドペーパーへの含浸性が低下して成形性が低下す
る場合がある。なお、熱硬化性樹脂組成物に複数の種類
の無機充填材を含有する場合、各々の重量比率に応じた
平均値をその平均粒子径とする。The thermosetting resin composition has a solid content of 1%.
It is important that 1 to 10 parts by weight of an inorganic filler having an average particle diameter of 1 to 10 μm is contained in 00 parts by weight. When the average particle size exceeds 10 μm, the amount of the inorganic filler adhering to the aramid paper surface is likely to be settled in the thermosetting resin composition because the inorganic filler tends to settle and a difference in the concentration of the inorganic filler easily occurs. And the effect of improving surface smoothness is difficult to obtain uniformly, and the average particle diameter is 1 μm.
If it is less than 1, the dispersibility of the inorganic filler in the thermosetting resin composition is poor, so if it is desired to uniformly disperse, it is necessary to lengthen the stirring time for mixing, or it is necessary to increase the stirring conditions for practical use. Not a target. When the ratio of the inorganic filler is less than 1 part by weight, the effect of improving the surface smoothness is small, and when it exceeds 10 parts by weight, the impregnation of the thermosetting resin composition into the aramid paper is reduced. In some cases, the formability may be reduced. When a plurality of types of inorganic fillers are contained in the thermosetting resin composition, the average value according to each weight ratio is defined as the average particle size.
【００１６】熱硬化性樹脂組成物中に適度な無機充填材
を含有すると、含有しない場合と比較して見かけの粘度
がやや大きくなるため、アラミドペーパー表面の低密度
の部分に熱硬化性樹脂組成物が保持されやすくなり、表
面平滑性が改良されると考えられる。また、アラミドペ
ーパー内部には無機充填材を除く熱硬化性樹脂組成物の
成分が含浸して良好な含浸性を有するため、成形性は低
下しにくいと考えられる。If the thermosetting resin composition contains an appropriate amount of inorganic filler, the apparent viscosity becomes slightly larger as compared with the case where the inorganic filler is not contained, so that the thermosetting resin composition is added to the low-density portion of the aramid paper surface. It is considered that the material is easily held and the surface smoothness is improved. Also, since the inside of the aramid paper is impregnated with the components of the thermosetting resin composition excluding the inorganic filler and has good impregnating properties, it is considered that the moldability is unlikely to deteriorate.
【００１７】なお、熱硬化性樹脂組成物に含有する無機
充填材は平均粒子径が１〜１０μｍである、Ｅガラス等
のガラス又はタルクの粉末である。Ｅガラスの粉末の場
合、ドリル加工性と耐熱性のバランスが良く好ましい。[0017] Incidentally, the inorganic filler contained in the thermosetting resin composition has an average particle size of 1 to 10 [mu] m, a glass or talc powder such as E glass. In the case of E glass powder, a good balance between drill workability and heat resistance is preferable.
【００１８】また、熱硬化性樹脂組成物中に含有するこ
とができる溶剤等としてはＮ，Ｎ−ジメチルホルムアミ
ド等のアミド類、エチレングリコールモノメチルエーテ
ル等のエーテル類、アセトン、メチルエチルケトン等の
ケトン類、メタノール、エタノール等のアルコール類、
ベンゼン、トルエン等の芳香族炭化水素類等が挙げられ
る。なお溶剤を含有する場合には、溶剤を除く熱硬化性
樹脂組成物固形分１００重量部に対して、平均粒子径が
１〜１０μｍの無機充填材を１〜１０重量部含有するこ
とが重要である。Examples of solvents which can be contained in the thermosetting resin composition include amides such as N, N-dimethylformamide; ethers such as ethylene glycol monomethyl ether; ketones such as acetone and methyl ethyl ketone; Alcohols such as methanol and ethanol,
Examples thereof include aromatic hydrocarbons such as benzene and toluene. When a solvent is contained, it is important to contain 1 to 10 parts by weight of an inorganic filler having an average particle diameter of 1 to 10 μm based on 100 parts by weight of the solid content of the thermosetting resin composition excluding the solvent. is there.
【００１９】本発明のプリプレグに用いられる基材とし
ては、アラミドペーパーに限定される。このアラミドペ
ーパーは、適当な長さのアラミドの繊維を必要に応じて
バインダーとともに抄紙した後、温度及び圧力をかけて
製造したものである。そしてアラミドは、ポリパラフェ
ニレンテレフタルアミドである。なお、ポリパラフェニ
レンテレフタルアミドのアラミドペーパーを用いた場
合、耐熱性が優れる。The substrate used in the prepreg of the present invention is limited to aramid paper. This aramid paper is manufactured by applying a temperature and a pressure after paper-making a suitable length of aramid fiber together with a binder as necessary. The aramid is polyparaphenylene terephthalamide. In the case of using the aramid paper polyparaphenylene terephthalamide, it is Ru excellent heat resistance.
【００２０】本発明の請求項４に係る積層板は、上述の
方法で得られたプリプレグを所要枚数重ねるとともに、
必要に応じて銅、アルミニウム、ニッケル等の金属箔を
その片側又は両側に配して積層した後、加熱加圧して成
形することにより得られる。In the laminated board according to a fourth aspect of the present invention, a required number of prepregs obtained by the above-described method are stacked,
If necessary, a metal foil of copper, aluminum, nickel or the like is arranged on one side or both sides thereof, laminated, and then formed by heating and pressing.
【００２１】表面平滑性が悪い、すなわち凹凸が大きい
プリプレグを積層すると、そのプリプレグの凹部に空気
を抱き込んで積層されるため、その積層物中に大量の空
気を含むことになり、加熱加圧して成形することにより
熱硬化性樹脂組成物を流動化させても積層物中の空気が
十分には除かれず、成形して得られる積層板中に気泡が
残留しやすくなるが、本発明の請求項４に係る積層板
は、本発明の請求項１〜３に係る表面平滑性が優れたプ
リプレグを用いているため、プリプレグとプリプレグ
や、プリプレグと金属箔等を積層したときその間に抱き
込む空気の量が少なくなり、成形すると気泡の残留が少
ない積層板となる。When a prepreg having poor surface smoothness, that is, a large unevenness is laminated, air is embraced in the concave portion of the prepreg and laminated, so that a large amount of air is contained in the laminate, and the laminate is heated and pressurized. Even if the thermosetting resin composition is fluidized by molding, air in the laminate is not sufficiently removed, and air bubbles are likely to remain in the laminate obtained by molding. Since the laminate according to claim 4 uses the prepreg having excellent surface smoothness according to claims 1 to 3 of the present invention, when the prepreg and the prepreg or the prepreg and the metal foil are laminated, they are embraced therebetween. The amount of air is reduced, and when molded, a laminated plate with less residual air bubbles is obtained.
【００２２】[0022]
（実施例１）熱硬化性樹脂組成物として、下記の熱硬化
性樹脂２種類、硬化剤、硬化促進剤、無機充填材及び溶
剤２種類よりなるエポキシ樹脂系樹脂組成物を使用し
た。なおこの場合の熱硬化性樹脂組成物固形分１００重
量部に対する無機充填材の比率は、４．９重量部とな
る。 ・熱硬化性樹脂１：エポキシ当量が２２０であるクレゾ
ールノボラック型エポキシ樹脂［東都化成社製、商品名
ＹＤＣＮ−２２０］を固形分として１０重量部 ・熱硬化性樹脂２：エポキシ当量が５００であるテトラ
ブロモビスフェノールＡ型エポキシ樹脂［東都化成社
製、商品名ＹＤＢ−５００］を固形分として３重量部 ・硬化剤：ジシアンジアミド（Ｄｉｃｙ）を０．５重量
部 ・硬化促進剤：ベンジルメチルアミンを０．２重量部 ・無機充填材：平均粒子径８μｍのＥガラスの粉末［日
東紡績社製、商品名ＰＦＡ−４５３］を０．７重量部 ・溶剤１：メチルエチルケトン（ＭＥＫ）を５０重量部 ・溶剤２：Ｎ，Ｎ−ジメチルホルムアミド（ＤＭＦ）を
６重量部。(Example 1) As a thermosetting resin composition, an epoxy resin-based resin composition comprising the following two thermosetting resins, a curing agent, a curing accelerator, an inorganic filler, and two solvents was used. In this case, the ratio of the inorganic filler to 100 parts by weight of the solid content of the thermosetting resin composition is 4.9 parts by weight. Thermosetting resin 1: 10 parts by weight of a cresol novolak type epoxy resin having an epoxy equivalent of 220 [YDCN-220, manufactured by Toto Kasei Co., Ltd.] as a solid content Thermosetting resin 2: Epoxy equivalent of 500 3 parts by weight of a tetrabromobisphenol A type epoxy resin [YDB-500, manufactured by Toto Kasei Co., Ltd.] as a solid content.-Curing agent: 0.5 parts by weight of dicyandiamide (Dicy)-Curing accelerator: 0 of benzylmethylamine 0.2 parts by weight ・ Inorganic filler: 0.7 parts by weight of E glass powder having an average particle diameter of 8 μm [trade name: PFA-453, manufactured by Nitto Boseki Co., Ltd.] ・ Solvent 1: 50 parts by weight of methyl ethyl ketone (MEK) ・ Solvent 2: 6 parts by weight of N, N-dimethylformamide (DMF).
【００２３】この熱硬化性樹脂組成物を、ポリパラフェ
ニレンテレフタルアミドよりなる単位面積当たりの重量
７２ｇ／平方ｃｍ、厚み１３０μｍのアラミドペーパー
［デュポン社製、商品名サーマウント］に、乾燥後の熱
硬化性樹脂組成物の量が、熱硬化性樹脂組成物及びアラ
ミドペーパーの合計１００重量部に対し、５４重量部と
なるように調整して含浸した後、最高温度１６５℃で乾
燥して厚み１４０μｍのプリプレグを作製した。This thermosetting resin composition was dried on aramid paper (trade name: Thermomount, manufactured by DuPont) having a weight per unit area of 72 g / square cm and a thickness of 130 μm, made of polyparaphenylene terephthalamide. The amount of the curable resin composition was adjusted to be 54 parts by weight with respect to the total of 100 parts by weight of the thermosetting resin composition and the aramid paper, and then impregnated. Was prepared.
【００２４】次いで、得られたプリプレグを２枚重ね、
さらにその両外側に厚み３５μｍの銅箔を配して積層し
た後、この積層物を金属プレートで挟み、最高温度１７
０℃、圧力３．０ＭＰａで１２０分加熱加圧して成形し
て両面銅張り積層板を得た。Next, two sheets of the obtained prepreg are stacked,
Further, after a copper foil having a thickness of 35 μm is arranged on both outer sides thereof and laminated, the laminate is sandwiched between metal plates, and a maximum temperature of 17 μm is applied.
The molded product was heated and pressed at 0 ° C. and a pressure of 3.0 MPa for 120 minutes to obtain a double-sided copper-clad laminate.
【００２５】（実施例２）熱硬化性樹脂組成物に配合す
る硬化剤として、フェノールノボラック樹脂を７重量部
用いたこと、及びベンジルメチルアミンの配合量を０．
５重量部としたこと、及びＥガラスの粉末の配合量を
１．０重量部としたこと以外は実施例１と同様にしてプ
リプレグ及び両面銅張り積層板を得た。なおこの場合の
熱硬化性樹脂組成物固形分１００重量部に対する無機充
填材の比率は、４．７重量部となる。Example 2 A phenol novolak resin was used in an amount of 7 parts by weight as a curing agent to be added to the thermosetting resin composition, and the amount of benzylmethylamine was 0.1%.
A prepreg and a double-sided copper-clad laminate were obtained in the same manner as in Example 1 except that the amount was 5 parts by weight and the amount of the E glass powder was 1.0 part by weight. In this case, the ratio of the inorganic filler to 100 parts by weight of the solid content of the thermosetting resin composition is 4.7 parts by weight.
【００２６】（実施例３）熱硬化性樹脂組成物に配合す
る硬化剤として、フェノールノボラック樹脂を７重量部
用いたこと、及びベンジルメチルアミンの配合量を０．
５重量部としたこと、及び無機充填材として平均粒子径
１．６μｍのタルク［日本タルク社製、商品名ミクロエ
ース Ｐ−４］を１．０重量部用いたこと以外は実施例
１と同様にしてプリプレグ及び両面銅張り積層板を得
た。なおこの場合の熱硬化性樹脂組成物固形分１００重
量部に対する無機充填材の比率は、４．７重量部とな
る。Example 3 A phenol novolak resin was used in an amount of 7 parts by weight as a curing agent to be added to the thermosetting resin composition, and the compounding amount of benzylmethylamine was 0.1%.
Same as Example 1 except that 5 parts by weight and 1.0 part by weight of talc (trade name: Micro Ace P-4, manufactured by Nippon Talc Co., Ltd.) having an average particle diameter of 1.6 μm were used as the inorganic filler. To obtain a prepreg and a double-sided copper-clad laminate. In this case, the ratio of the inorganic filler to 100 parts by weight of the solid content of the thermosetting resin composition is 4.7 parts by weight.
【００２７】（実施例４）熱硬化性樹脂組成物として、
下記の熱硬化性樹脂、硬化剤、無機充填材及び溶剤より
なるポリイミド樹脂系樹脂組成物を使用した。なおこの
場合の熱硬化性樹脂組成物固形分１００重量部に対する
無機充填材の比率は、５．２重量部となる。 ・熱硬化性樹脂：ビスマレイミドを４０重量部 ・硬化剤：４，４’−ジアミノジフェニルメタンを１５
重量部 ・無機充填材：平均粒子径８μｍのＥガラスの粉末［日
東紡績社製、商品名ＰＦＡ−４５３］を３重量部 ・溶剤：Ｎ，Ｎ−ジメチルホルムアミドを３０重量部。Example 4 As a thermosetting resin composition,
A polyimide resin-based resin composition comprising the following thermosetting resin, curing agent, inorganic filler and solvent was used. In this case, the ratio of the inorganic filler to 100 parts by weight of the solid content of the thermosetting resin composition is 5.2 parts by weight. -Thermosetting resin: 40 parts by weight of bismaleimide-Curing agent: 15 of 4,4'-diaminodiphenylmethane
Parts by weight-Inorganic filler: 3 parts by weight of E glass powder [trade name: PFA-453, manufactured by Nitto Boseki Co., Ltd.] having an average particle diameter of 8 µm-Solvent: 30 parts by weight of N, N-dimethylformamide.
【００２８】このポリイミド樹脂系樹脂組成物を用いた
こと、及び成形の温度を２００℃としたこと以外は実施
例１と同様にしてプリプレグ及び両面銅張り積層板を得
た。A prepreg and a double-sided copper-clad laminate were obtained in the same manner as in Example 1 except that this polyimide resin-based resin composition was used and the molding temperature was set to 200 ° C.
【００２９】（実施例５）熱硬化性樹脂組成物に配合す
る無機充填材として平均粒子径１．６μｍのタルク［日
本タルク社製、商品名ミクロエース Ｐ−４］を３重量
部用いたこと以外は実施例４と同様にしてプリプレグ及
び両面銅張り積層板を得た。なおこの場合の熱硬化性樹
脂組成物固形分１００重量部に対する無機充填材の比率
は、５．２重量部となる。Example 5 3 parts by weight of talc having an average particle size of 1.6 μm [Microace P-4, trade name, manufactured by Nippon Talc Co., Ltd.] was used as an inorganic filler to be mixed in the thermosetting resin composition. Except for the above, a prepreg and a double-sided copper-clad laminate were obtained in the same manner as in Example 4. In this case, the ratio of the inorganic filler to 100 parts by weight of the solid content of the thermosetting resin composition is 5.2 parts by weight.
【００３０】（比較例１）熱硬化性樹脂組成物に配合す
るＥガラスの粉末の量を０．１重量部としたこと以外は
実施例１と同様にしてプリプレグ及び両面銅張り積層板
を得た。なおこの場合の熱硬化性樹脂組成物固形分１０
０重量部に対する無機充填材の比率は、０．７重量部と
なる。(Comparative Example 1) A prepreg and a double-sided copper-clad laminate were obtained in the same manner as in Example 1 except that the amount of the E glass powder to be added to the thermosetting resin composition was 0.1 part by weight. Was. In this case, the thermosetting resin composition solid content 10
The ratio of the inorganic filler to 0 parts by weight is 0.7 parts by weight.
【００３１】（比較例２）熱硬化性樹脂組成物に配合す
るＥガラスの粉末の量を２．０重量部としたこと以外は
実施例１と同様にしてプリプレグ及び両面銅張り積層板
を得た。なおこの場合の熱硬化性樹脂組成物固形分１０
０重量部に対する無機充填材の比率は、１２．７重量部
となる。(Comparative Example 2) A prepreg and a double-sided copper-clad laminate were obtained in the same manner as in Example 1 except that the amount of the E glass powder to be added to the thermosetting resin composition was 2.0 parts by weight. Was. In this case, the thermosetting resin composition solid content 10
The ratio of the inorganic filler to 0 parts by weight is 12.7 parts by weight.
【００３２】（比較例３）熱硬化性樹脂組成物に配合す
るＥガラスとして平均粒子径２５μｍのＥガラスの粉末
［日東紡績社製、商品名ＰＦＡ−４０３］を用いたこと
以外は実施例１と同様にしてプリプレグ及び両面銅張り
積層板を得た。Comparative Example 3 Example 1 was repeated except that E glass powder having an average particle diameter of 25 μm [trade name: PFA-403, manufactured by Nitto Boseki Co., Ltd.] was used as the E glass to be mixed with the thermosetting resin composition. In the same manner as in the above, a prepreg and a double-sided copper-clad laminate were obtained.
【００３３】（評価、結果）実施例１〜５及び比較例１
〜３で得られたプリプレグについて表面粗度を測定し
た。測定方法は、表面粗さ計［東京精密株式会社製、サ
ーフコム］を用いて、ＪＩＳ規格Ｂ０６０１に従い測定
した。(Evaluation and Results) Examples 1 to 5 and Comparative Example 1
The surface roughness was measured for the prepregs obtained in Nos. 1 to 3. The measurement method was measured using a surface roughness meter [Surfcom manufactured by Tokyo Seimitsu Co., Ltd.] in accordance with JIS B0601.
【００３４】また、実施例１〜５及び比較例１〜３で得
られた両面銅張り積層板について、成形性、比誘電率及
び誘電正接を測定した。成形性は表面の銅箔をエッチン
グで除去した後、内部に気泡が残留していることにより
白色化している等の異常の有無を目視により評価し、○
は白色化している等の異常の発生が無し、△は白色化し
ている等の異常の発生が部分的に発生、×は白色化して
いる等の異常の発生が全体的に発生とした。比誘電率及
び誘電正接は、ＪＩＳ規格Ｃ６４８１に従い１ＭＨｚで
測定した。With respect to the double-sided copper-clad laminates obtained in Examples 1 to 5 and Comparative Examples 1 to 3, formability, relative permittivity and dielectric loss tangent were measured. Formability was evaluated by visually inspecting for abnormalities such as whitening due to bubbles remaining inside after removing the copper foil on the surface by etching.
Indicates no occurrence of abnormality such as whitening, Δ indicates partial occurrence of abnormality such as whitening, and x indicates occurrence of abnormality such as whitening as a whole. The relative permittivity and the dielectric loss tangent were measured at 1 MHz according to JIS standard C6481.
【００３５】結果は表１及び表２に示した通り、各実施
例で得られたプリプレグは各比較例で得られたプリプレ
グと比べ表面粗度が良好であることが確認された。ま
た、各実施例で得られた両面銅張り積層板は各比較例で
得られた両面銅張り積層板と比べ成形性が良好であるこ
とが確認された。As shown in Tables 1 and 2, it was confirmed that the prepreg obtained in each of the examples had better surface roughness than the prepreg obtained in each of the comparative examples. In addition, it was confirmed that the double-sided copper-clad laminate obtained in each example had better moldability than the double-sided copper-clad laminate obtained in each comparative example.
【００３６】[0036]
【表１】 [Table 1]
【００３７】[0037]
【表２】 [Table 2]
【００３８】[0038]
【発明の効果】本発明の請求項１から請求項３に係るプ
リプレグは、熱硬化性樹脂組成物固形分１００重量部に
対し、平均粒子径が１〜１０μｍの無機充填材を１〜１
０重量部含有する熱硬化性樹脂組成物をアラミドペーパ
ーに含浸してなるため、表面平滑性が優れたプリプレグ
となる。The prepreg according to any one of claims 1 to 3 of the present invention comprises an inorganic filler having an average particle diameter of 1 to 10 μm and a solid content of 100 to 100 parts by weight of the thermosetting resin composition.
Since aramid paper is impregnated with a thermosetting resin composition containing 0 parts by weight, a prepreg having excellent surface smoothness is obtained.
【００３９】本発明の請求項４に係る積層板は、本発明
の請求項１〜３に係る表面平滑性が優れたプリプレグを
用いているため、プリプレグと金属箔等を積層したとき
その間に抱き込む空気の量が少なくなり、気泡の残留が
少ない積層板となる。The laminate according to claim 4 of the present invention uses the prepreg having excellent surface smoothness according to claims 1 to 3 of the present invention. The amount of air to be introduced is reduced, and a laminate having less air bubbles is obtained.
───────────────────────────────────────────────────── フロントページの続き (51)Int.Cl.7 識別記号 ＦＩ Ｂ２９Ｌ 9:00 Ｃ０８Ｌ 63:00 Ｃ０８Ｌ 63:00 Ｂ２９Ｃ 67/14 Ｇ (56)参考文献 特開 平１−118539（ＪＰ，Ａ) 特開 平３−296535（ＪＰ，Ａ) 特開 平７−324141（ＪＰ，Ａ) 特開 昭58−94456（ＪＰ，Ａ) 特開 昭62−270333（ＪＰ，Ａ) 特開 平７−133359（ＪＰ，Ａ) 特開 平２−194588（ＪＰ，Ａ) 特開 平４−268765（ＪＰ，Ａ) 特開 平１−194499（ＪＰ，Ａ) (58)調査した分野(Int.Cl.7，ＤＢ名) C08J 5/24 B32B 15/08 ────────────────────────────────────────────────── ─── Continued on the front page (51) Int.Cl. 7 Identification symbol FI B29L 9:00 C08L 63:00 C08L 63:00 B29C 67/14 G (56) References JP-A 1-118539 (JP, A JP-A-3-296535 (JP, A) JP-A-7-324141 (JP, A) JP-A-58-94456 (JP, A) JP-A-62-270333 (JP, A) 133359 (JP, A) JP-A-2-194588 (JP, A) JP-A-4-268765 (JP, A) JP-A-1-194499 (JP, A) (58) Fields investigated (Int. Cl. 7 , DB name) C08J 5/24 B32B 15/08
Claims (4)
に対し、平均粒子径が１〜１０μｍの無機充填材であっ
て、ガラスの粉末又はタルクの粉末である無機充填材を
１〜１０重量部含有する熱硬化性樹脂組成物を、ポリパ
ラフェニレンテレフタルアミドであるアラミドの繊維を
抄紙して製造しているアラミドペーパーに含浸してなる
ことを特徴とするプリプレグ。To 1. A thermosetting resin composition 100 parts by weight of the solid content, average particle diameter encounters 1~10μm inorganic filler
A thermosetting resin composition containing 1 to 10 parts by weight of an inorganic filler which is a powder of glass or a powder of talc ;
Aramid fiber which is raphenylene terephthalamide
A prepreg characterized by being impregnated into aramid paper manufactured by papermaking .
ることを特徴とする請求項１記載のプリプレグ。2. The prepreg according to claim 1, wherein the inorganic filler contains E glass powder.
樹脂組成物であることを特徴とする請求項１又は請求項
２記載のプリプレグ。3. The prepreg according to claim 1, wherein the thermosetting resin composition is an epoxy resin-based resin composition.
のプリプレグを用いて成形してなることを特徴とする積
層板。4. A laminate formed by using the prepreg according to any one of claims 1 to 3.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP10673496A JP3322123B2 (en) | 1996-04-26 | 1996-04-26 | Prepreg and laminate using the same |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP10673496A JP3322123B2 (en) | 1996-04-26 | 1996-04-26 | Prepreg and laminate using the same |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH09291160A JPH09291160A (en) | 1997-11-11 |
| JP3322123B2 true JP3322123B2 (en) | 2002-09-09 |
Family
ID=14441168
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP10673496A Expired - Fee Related JP3322123B2 (en) | 1996-04-26 | 1996-04-26 | Prepreg and laminate using the same |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3322123B2 (en) |
Families Citing this family (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP4137625B2 (en) * | 2002-12-20 | 2008-08-20 | 日本化薬株式会社 | Polyimide precursor composition |
| TWI633741B (en) * | 2012-03-07 | 2018-08-21 | 日商杜邦帝人先進紙股份有限公司 | Reel for motor, manufacturing method thereof, motor using the same, motor generator and generator |
-
1996
- 1996-04-26 JP JP10673496A patent/JP3322123B2/en not_active Expired - Fee Related
Also Published As
| Publication number | Publication date |
|---|---|
| JPH09291160A (en) | 1997-11-11 |
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