JP4171952B2 - Thermosetting resin composition, prepreg, laminate and printed wiring board - Google Patents
Thermosetting resin composition, prepreg, laminate and printed wiring board Download PDFInfo
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- JP4171952B2 JP4171952B2 JP33221799A JP33221799A JP4171952B2 JP 4171952 B2 JP4171952 B2 JP 4171952B2 JP 33221799 A JP33221799 A JP 33221799A JP 33221799 A JP33221799 A JP 33221799A JP 4171952 B2 JP4171952 B2 JP 4171952B2
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- prepreg
- printed wiring
- wiring board
- thermosetting resin
- resin composition
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Description
【0001】
【発明の属する技術分野】
本発明は、熱硬化性樹脂組成物、プリプレグ、積層板及びプリント配線板に関する。
【0002】
【従来の技術】
プリント配線板は、繊維基材に熱硬化性樹脂組成物のワニスを含浸乾燥してなるプリプレグを1枚または所要枚数重ねた構成体を加熱加圧成形して積層板を得、この積層板を基板として、その表面に回路を形成して製造される。
通常、積層板を製造するときに銅はくなど金属はくなどを同時に重ねて金属はく張り積層板とし、この金属はくをエッチングして回路を形成している。
【0003】
近年、半導体搭載用パッケージ.などの用途に用いられるプリント配線板の基板は黒色を基調とするものが主流となっている。それは、ワイヤボンディングの良否判定が容易になること、外観的に高級感が得られること、及び露光工程において紫外線が反対面に透過して反対面にあるレジストが感光していわゆる裏ぼけをおこすのを防ぐためである。
基板を黒色とする手法としては、積層板を製造するためのプリプレグに黒色の繊維基材を用いる手法や、熱硬化性樹脂組成物にカーボンブラック、スピリットブラックなどのカーボン系顔料を配合する手法が知られている。
【発明が解決しようとする課題】
【0004】
ところが、黒色の繊維基材を用いて基板を黒色とする手法では、繊維基材に隙間があるため必ずしも十分な紫外線遮蔽性が得られず、また繊維基材が十分な黒さを有していない場合があり外観上の問題もあった。
また、熱硬化性樹脂組成物にカーボンブラック、スピリットブラック等のカーボン系顔料を配合する手法では、カーボン自体が導電性を有するために基板の絶縁性低下、及び電食による回路間の絶縁低下を生じやすかった。このためプリント配線板としての信頼性(以下単に信頼性とする)が低下するという問題があった。
【0005】
本発明は、かかる実状に鑑みなされたもので、請求項1に記載の発明は、紫外線を十分に遮蔽することができ、絶縁性及び信頼性の低下がない積層板を製造するために好適な熱硬化性樹脂組成物を提供することを目的とする。
請求項2に記載の発明は、プリント配線板として絶縁性及び信頼性の低下がない積層板を製造するために好適なプリプレグを提供することを目的とする。
請求項3に記載の発明は、プリント配線板として絶縁性及び信頼性の低下がない積層板を提供することを目的とする。
請求項4に記載の発明は、絶縁性及び信頼性の低下がないプリント配線板を提供することを目的とする。
【0006】
【課題を解決するための手段】
すなわち、本発明は、下記構造式で示される黒色染料を含有してなるプリプレグ用熱硬化性樹脂組成物を用いたプリプレグ、積層板及びプリント配線板に関する。
【化2】
【0007】
【発明の実施の形態】
構造式が化2で示される化合物は、ソルベントブラック3として知られている黒色染料であり、この染料は市販品を使用することができる。市販品としては、中央合成化学株式会社からChuo Sudan Black141という商品名で市販されているものなどを挙げることができる。
【0008】
熱硬化性樹脂組成物のべースとなる熱硬化性樹脂としては、積層板製造において汎用されている熱硬化性樹脂を用いることができ特に制限はない。例えば、エポキシ樹脂、ビスマレイミド樹脂、ポリイミド樹脂、フェノール樹脂、不飽和ポリエステル樹脂などを挙げられる。
なかでも、エポキシ樹脂が好ましく用いられる。エポキシ樹脂としては、分子内に2個以上のエポキシ基を持つ化合物であればよく、例えばフェノール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、レゾール型エポキシ樹脂、ビスフェノール型エポキシ樹脂などのフェノール類のグリシジルエーテルであるエポキシ樹脂(フェノール型エポキシ樹脂)や、脂環式エポキシ樹脂、エポキシ化ポリブタジエン、グリシジルエステル型エポキシ樹脂、グリシジルアミン型エポキシ樹脂、イソシアヌレート型エポキシ樹脂、可とう性エポキシ樹脂などが挙げられる。これらの多官能エポキシ樹脂は、単独で用いてもよく、2種類以上を併用してもよい。
【0009】
熱硬化性エポキシ樹脂としてエポキシ樹脂を用いたときには、エポキシ樹脂を硬化させるため、硬化剤及び硬化促進剤が配合される。硬化剤としては、ノボラック型フェノール樹脂、ジシアンジアミド、酸無水物、アミン類などが挙げられ、硬化促進剤としては、イミダゾール類などが挙げられる。これらは単独で用いてもよく、2種類以上併用してもよい。また、硬化剤及び硬化促進剤は用いられる多官能エポキシ樹脂の量に応じて必要とされる範囲で配合される。
硬化剤は、エポキシ樹脂のエポキシ基1当量に対して、硬化剤の官能基が0.8〜1.2当量の範囲となるように配合されるのが好ましく、0.80〜1.1当量の範囲となるように配合されるのがより好ましい。硬化剤の官能基が0.8当量未満の場合、及び1.2当量を超えるいずれの場合も、ガラス転移点が低くなり、吸湿しやすくなるため、はんだ耐熱性が低下する傾向にある。
また、硬化促進剤としては従来公知の種々のものを使用することができ、特に制限はない。例えば熱硬化性樹脂としてエポキシ樹脂を用いる場合には、イミダゾール系化合物、有機リン系作合物、第3級アミン、第4級アンモニウム塩などが挙げられる。これら硬化促進剤は、単独で使用してもよく、2種類以上を併用してもよい。
熱硬化性樹脂、必要により配合される硬化剤のほか、機械特性改善、増量による原価低減などの観点から無機充填剤を配合することもできる。このような無機充填剤としては、アルミナ・微粉末シリカ、水酸化アルミニウム、ケイ酸ジルコニウム、タルクなどが挙げられる。
【0010】
化2で示される黒色染料の配合量は、熱硬化性樹脂組成物中に0.01〜2重量%、好ましくは0.1〜1重量%の範囲とするのが好ましい。2重量%を超えて多量に配合しても効果は変わらない。
【0011】
本発明になる熱硬化性樹脂組成物は、ワニスとして繊維基材に含浸乾燥してプリプレグとされる。ワニスとするときに用いられる溶剤は、用いられる熱硬化性樹脂を溶解可能な従来公知の溶剤を用いることができ特に制限はない。液状の熱硬化性樹脂を用いる場合には無溶剤とすることもできる。
溶剤としては、例えば、水、メタノール、エタノール、プロピルアルコール、ブチルアルコール、アセトン、メチルエチルケトン、トルエン、キシレン、ジオキサン、N、Nジメチルホルムアミド、エチレングリコールモノメチルエーテル、エチレングリコールモノメチルエーテルなどが挙げられ、これらの溶剤は単独で使用してもよく、また必要に応じて組み合わせて使用することもできる。
【0012】
本発明に用いられる繊維基材は、積層板製造において汎用されている繊維基材を用いることができ特に制限はないが、耐熱性など特性面から、ガラス織布またはガラス不織布が好ましく用いられる。
【0013】
繊維基材に熱硬化性樹脂組成物ワニスを含浸乾燥してプリプレグとするときの方法及び製造条件については、べ一スとなる熱硬化性樹脂について従来公知の方法及び条件によることができ特に制限はない。
また、得られたプリプレグは、一枚で又は複数枚を重ね、その片面又は両面に金属箔を重ね、温度150℃〜200℃、圧力1.0〜8.0MPa程度の範囲で加熱加圧して金属はく張り積層板とされる。金属はく張積層板に回路加工を施してプリント配線板を製造するときの方法については特に制約はなく公知の方法を用いることができる。
【0014】
積層板を製造するときの材料構成において、プリプレグを複数枚使用するときは、紫外線遮断の観点からは本発明のプリプレグを少なくとも1枚使用すればよい。また、本発明のプリプレグを配置する位置については特に制限はない。しかしながら、ワイヤボンディングの良否識別の容易さや外観上から、本発明になるプリプレグが最外層となるように構成するのが好ましい。
【0015】
【実施例】
実施例1
エポキシ当量480のブロム化エポキシ樹脂(東都化成(株)製、YDB−400(商品名))100部(重量部、以下同じ)、ジシアンジアミド3部、2−エチル−4−メチルイミダゾール0.17部及び構造式が化2で示される化合物(中央合成化学(株)製、商品名:Chuo Sudan Black141)0.5部を、エチレングリコールモノメチルエーテル25部、N、Nジメチルホルムアミド25部からなる溶剤に溶解することによりエポキシ樹脂組成物ワニスを調製した。
調製したエポキシ樹脂組成物ワニスを厚さ0.1mm、坪量104g/m2のガラス織布(日東紡績(株)製、GA−7010S136(商品名))に含浸乾燥後の付着量が50重量%になるように含浸、乾燥してプリプレグを作成した。
作製したプリプレグを2枚重ね、その両面に厚さ18μmの銅はくを置き、温度175℃圧力3MPaで減圧下に60分間加熱加圧して両面銅張積層板を作製し、作製した両面銅張積層板にエッチングを施して回路を形成することにより両面プリント配線板を得た。
得られた両面プリント配線板は、基板の外観が黒色を基調としており、ワイヤボンディングの良否識別が容易であった。
【0016】
比較例1
着色剤としてカーボンブラックを使用したほかは、実施例1と同様にして、エポキシ樹脂組成物ワニスを調製し、プリプレグを作製し両面プリント配線板を作製した。作製した両面プリント配線板は、外観が黒色を基調としておりワイヤボンディングの良否識別が容易であったが、耐電食性に劣っていた。
【0017】
比較例2
構造式が化2で示される化合物を配合しないほかは、実施例1と同様にして、エポキシ樹脂組成物ワニスを調製した。
このワニスを厚さ0.1mm、坪量104g/m2の黒色系ガラス織布(日東紡績(株)製、GA−7010XB07(商品名))に含浸、乾燥したほかは実施例1と同様にして、プリプレグを作製し両面プリント配線板を作製した。
作製した両面プリント配線板は、外観が黒色を基調としており、ワイヤボンディングの良否識別が容易であったが、基板の紫外線透過率が大であった。
【0018】
なお、紫外線透過率は、両面銅張積層板の銅箔をエッチングにより全面除去し、これに紫外線を照射して透過率を調べた。また、耐電食性は、両面銅張積層板に穴間距離300μmまたは200μm、穴径Φ0.5の電気めっき100穴で表裏の回路を電気的に接続した回路パターン2回路を形成し、温度85℃、相対湿度85%の恒温恒湿槽中にてこの2回路間に直流100Vの電圧を1000時間印加した。その後の2回路間の絶縁抵抗を測定することにより耐電食性を調べた。
これらの結果を表1に示した。
【0019】
【表1】
【0020】
表1から、構造式が化2で示される化合物を配合した実施例1では積層板の紫外線透過率が小さく、また、プリント配線板の電食による絶縁低下が無いことから信頼性が良好であることが示される。これに対してカーボン系顔料を配合した比較例1においては紫外線透過率は小さいものの、電食による絶縁低下が大きいことから信頼性がよくないことが示される。また、黒色系ガラス織布を用いた比較例2においては、耐電食性が良好であるものの紫外線透過率が大きいことが示される。
【0021】
【発明の効果】
本発明によれば、紫外線を十分に遮蔽することができ、かつ、黒色を基調とする積層板をを得ることができる。そしてこの積層板は紫外線遮蔽性が良好であることから、両面同時露光によりプリント配線板とすることができ、また、ワイヤボンディングの良否識別も容易で、電食による絶縁低下がないことから信頼性に優れたプリント配線板を提供することができる。[0001]
BACKGROUND OF THE INVENTION
The present invention relates to a thermosetting resin composition, a prepreg, a laminated board, and a printed wiring board.
[0002]
[Prior art]
A printed wiring board is obtained by heat-pressing a structure in which a prepreg formed by impregnating and drying a varnish of a thermosetting resin composition on a fiber base material and drying is obtained to obtain a laminated board. A substrate is manufactured by forming a circuit on the surface thereof.
Usually, when manufacturing a laminated board, metal foils, such as copper foil, are overlapped simultaneously to form a metal-laminated laminated board, and the metal foil is etched to form a circuit.
[0003]
In recent years, substrates of printed wiring boards used for applications such as semiconductor mounting packages have been mainly based on black. It is easy to judge the quality of wire bonding, high-quality appearance is obtained, and in the exposure process, ultraviolet rays are transmitted to the opposite surface and the resist on the opposite surface is exposed to cause so-called blurring. Is to prevent.
As a method of making the substrate black, there are a method of using a black fiber base material for a prepreg for manufacturing a laminate, and a method of blending a carbon-based pigment such as carbon black or spirit black into a thermosetting resin composition. Are known.
[Problems to be solved by the invention]
[0004]
However, in the method of making the substrate black using a black fiber base material, there is a gap in the fiber base material, so that sufficient UV shielding is not always obtained, and the fiber base material has sufficient blackness. There were cases where there were no appearance problems.
In addition, in the method of blending carbon pigments such as carbon black and spirit black into the thermosetting resin composition, the carbon itself has conductivity, so that the insulation of the substrate is lowered and the insulation between the circuits due to electrolytic corrosion is reduced. It was easy to occur. For this reason, there has been a problem that reliability as a printed wiring board (hereinafter simply referred to as reliability) is lowered.
[0005]
The present invention has been made in view of such a situation, and the invention according to claim 1 is suitable for manufacturing a laminated board that can sufficiently shield ultraviolet rays and does not have a decrease in insulation and reliability. It aims at providing a thermosetting resin composition.
An object of the present invention is to provide a prepreg suitable for manufacturing a laminated board having no deterioration in insulation and reliability as a printed wiring board.
It is an object of the present invention to provide a laminated board having no deterioration in insulation and reliability as a printed wiring board.
An object of the present invention is to provide a printed wiring board which does not have a decrease in insulation and reliability.
[0006]
[Means for Solving the Problems]
That is, the present invention relates to a prepreg, a laminate and a printed wiring board using a thermosetting resin composition for prepregs containing a black dye represented by the following structural formula.
[Chemical 2]
[0007]
DETAILED DESCRIPTION OF THE INVENTION
The compound represented by the chemical formula 2 is a black dye known as Solvent Black 3, and a commercial product can be used as this dye. As a commercial item, what is marketed with the brand name Chuo Sudan Black141 from Chuo Synthetic Chemical Co., Ltd. can be mentioned.
[0008]
As the thermosetting resin used as the base of the thermosetting resin composition, a thermosetting resin widely used in the production of laminates can be used, and there is no particular limitation. For example, an epoxy resin, a bismaleimide resin, a polyimide resin, a phenol resin, an unsaturated polyester resin, and the like can be given.
Among these, an epoxy resin is preferably used. The epoxy resin may be a compound having two or more epoxy groups in the molecule. For example, phenolic glycidyl such as phenol novolac type epoxy resin, cresol novolac type epoxy resin, resol type epoxy resin, bisphenol type epoxy resin, etc. Examples include ether epoxy resins (phenolic epoxy resins), cycloaliphatic epoxy resins, epoxidized polybutadiene, glycidyl ester epoxy resins, glycidylamine epoxy resins, isocyanurate epoxy resins, flexible epoxy resins, etc. . These polyfunctional epoxy resins may be used alone or in combination of two or more.
[0009]
When an epoxy resin is used as the thermosetting epoxy resin, a curing agent and a curing accelerator are blended to cure the epoxy resin. Examples of the curing agent include novolac type phenol resins, dicyandiamide, acid anhydrides, amines, and examples of the curing accelerator include imidazoles. These may be used alone or in combination of two or more. Moreover, a hardening | curing agent and a hardening accelerator are mix | blended in the required range according to the quantity of the polyfunctional epoxy resin used.
The curing agent is preferably blended so that the functional group of the curing agent is in the range of 0.8 to 1.2 equivalents relative to 1 equivalent of the epoxy group of the epoxy resin, 0.80 to 1.1 equivalents It is more preferable that they are blended in such a range. In both cases where the functional group of the curing agent is less than 0.8 equivalent and more than 1.2 equivalent, the glass transition point becomes low and moisture absorption tends to occur, so the solder heat resistance tends to decrease.
Moreover, conventionally well-known various things can be used as a hardening accelerator, and there is no restriction | limiting in particular. For example, when an epoxy resin is used as the thermosetting resin, an imidazole compound, an organic phosphorus compound, a tertiary amine, a quaternary ammonium salt, and the like can be given. These curing accelerators may be used alone or in combination of two or more.
In addition to thermosetting resins and curing agents blended as necessary, inorganic fillers can be blended from the viewpoints of improving mechanical properties and reducing costs by increasing the amount. Examples of such inorganic fillers include alumina / fine powder silica, aluminum hydroxide, zirconium silicate, and talc.
[0010]
The compounding amount of the black dye represented by Chemical Formula 2 is 0.01 to 2% by weight, preferably 0.1 to 1% by weight in the thermosetting resin composition. The effect does not change even if it is added in a large amount exceeding 2% by weight.
[0011]
The thermosetting resin composition according to the present invention is impregnated and dried into a fiber base material as a varnish to form a prepreg. As the solvent used for the varnish, a conventionally known solvent capable of dissolving the thermosetting resin to be used can be used, and there is no particular limitation. When a liquid thermosetting resin is used, it can be made solvent-free.
Examples of the solvent include water, methanol, ethanol, propyl alcohol, butyl alcohol, acetone, methyl ethyl ketone, toluene, xylene, dioxane, N, N dimethylformamide, ethylene glycol monomethyl ether, ethylene glycol monomethyl ether, and the like. A solvent may be used independently and can also be used in combination as needed.
[0012]
The fiber base material used in the present invention can be a fiber base material widely used in the production of laminates, and is not particularly limited, but a glass woven fabric or a glass nonwoven fabric is preferably used from the viewpoint of characteristics such as heat resistance.
[0013]
Regarding the method and production conditions when impregnating and drying a thermosetting resin composition varnish on a fiber base material to produce a prepreg, the base thermosetting resin can be based on conventionally known methods and conditions, and is particularly limited. There is no.
In addition, the obtained prepreg is a single sheet or a plurality of sheets, and a metal foil is stacked on one or both sides of the prepreg, and is heated and pressed in a temperature range of 150 ° C. to 200 ° C. and a pressure of about 1.0 to 8.0 MPa. A metal-laminated laminate is used. There are no particular restrictions on the method for producing a printed wiring board by subjecting a metal-clad laminate to circuit processing, and a known method can be used.
[0014]
When using a plurality of prepregs in the material configuration when manufacturing a laminated plate, at least one prepreg of the present invention may be used from the viewpoint of ultraviolet blocking. Moreover, there is no restriction | limiting in particular about the position which arrange | positions the prepreg of this invention. However, it is preferable to configure the prepreg according to the present invention to be the outermost layer from the viewpoint of easy and good identification of wire bonding and appearance.
[0015]
【Example】
Example 1
Brominated epoxy resin having an epoxy equivalent of 480 (manufactured by Tohto Kasei Co., Ltd., YDB-400 (trade name)) 100 parts (parts by weight, the same applies hereinafter), 3 parts of dicyandiamide, 0.17 parts of 2-ethyl-4-methylimidazole And 0.5 parts of a compound represented by the chemical formula (Chuo Synthetic Chemical Co., Ltd., trade name: Chuo Sudan Black 141) in a solvent comprising 25 parts of ethylene glycol monomethyl ether and 25 parts of N, N dimethylformamide. An epoxy resin composition varnish was prepared by dissolving.
The epoxy resin composition varnish thus prepared was impregnated and dried on a glass woven fabric (manufactured by Nitto Boseki Co., Ltd., GA-7010S136 (trade name)) having a thickness of 0.1 mm and a basis weight of 104 g / m 2. A prepreg was prepared by impregnation and drying to a percentage of 50%.
Two sheets of the prepared prepreg are stacked, 18 μm thick copper foil is placed on both sides of the prepreg, and a double-sided copper-clad laminate is prepared by heating and pressing at a temperature of 175 ° C. under a pressure of 3 MPa for 60 minutes. A double-sided printed wiring board was obtained by etching the laminated board to form a circuit.
In the obtained double-sided printed wiring board, the appearance of the substrate was based on black, and the quality of wire bonding was easy to identify.
[0016]
Comparative Example 1
An epoxy resin composition varnish was prepared in the same manner as in Example 1 except that carbon black was used as a colorant, and a prepreg was prepared to prepare a double-sided printed wiring board. The produced double-sided printed wiring board was based on black in appearance, and it was easy to identify the quality of wire bonding, but it was inferior in electric corrosion resistance.
[0017]
Comparative Example 2
An epoxy resin composition varnish was prepared in the same manner as in Example 1 except that the compound represented by the chemical formula 2 was not added.
This varnish was impregnated into a black glass woven fabric having a thickness of 0.1 mm and a basis weight of 104 g / m 2 (manufactured by Nitto Boseki Co., Ltd., GA-7010XB07 (trade name)) and dried in the same manner as in Example 1. Thus, a prepreg was produced to produce a double-sided printed wiring board.
The produced double-sided printed wiring board was based on black in appearance, and it was easy to identify the quality of wire bonding, but the substrate had a large ultraviolet transmittance.
[0018]
The ultraviolet transmittance was examined by removing the entire surface of the copper foil of the double-sided copper-clad laminate by etching and irradiating it with ultraviolet rays. In addition, with respect to electric corrosion resistance, a double-sided copper-clad laminate has a circuit pattern of 2 circuits in which the front and back circuits are electrically connected by electroplating 100 holes with a hole distance of 300 μm or 200 μm and a hole diameter of Φ0.5, and the temperature is 85 ° C. A voltage of 100 V DC was applied between these two circuits for 1000 hours in a constant temperature and humidity chamber having a relative humidity of 85%. The electrical corrosion resistance was examined by measuring the insulation resistance between the subsequent two circuits.
These results are shown in Table 1.
[0019]
[Table 1]
[0020]
From Table 1, in Example 1 in which a compound represented by the chemical formula 2 was blended, the ultraviolet transmission of the laminated board was small, and the insulation was not lowered due to the electrolytic corrosion of the printed wiring board, so the reliability was good. Is shown. On the other hand, in Comparative Example 1 in which a carbon pigment was blended, although the ultraviolet transmittance was small, it was shown that the reliability was not good because the insulation decrease due to electrolytic corrosion was large. Moreover, in the comparative example 2 using a black-type glass woven fabric, although the electrical corrosion resistance is favorable, it is shown that the ultraviolet-ray transmittance is large.
[0021]
【The invention's effect】
According to the present invention, it is possible to obtain a laminated board that can sufficiently block ultraviolet rays and is based on black. And because this laminated board has good UV shielding properties, it can be made into a printed wiring board by double-sided simultaneous exposure, and it is easy to identify the quality of wire bonding, and there is no insulation deterioration due to electrolytic corrosion, so it is reliable An excellent printed wiring board can be provided.
Claims (3)
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JP33221799A JP4171952B2 (en) | 1999-11-24 | 1999-11-24 | Thermosetting resin composition, prepreg, laminate and printed wiring board |
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JP33221799A JP4171952B2 (en) | 1999-11-24 | 1999-11-24 | Thermosetting resin composition, prepreg, laminate and printed wiring board |
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JP2001152032A JP2001152032A (en) | 2001-06-05 |
JP4171952B2 true JP4171952B2 (en) | 2008-10-29 |
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JP5265844B2 (en) * | 2004-11-16 | 2013-08-14 | 日立化成株式会社 | Thermosetting resin composition, prepreg, laminate and printed wiring board |
JP5169155B2 (en) * | 2007-11-08 | 2013-03-27 | 住友ベークライト株式会社 | Method for producing resin composition |
CN102223759A (en) * | 2010-04-14 | 2011-10-19 | 江阴市明康绝缘玻纤有限公司 | Phenolic paper-based light shielding single-sided copper-cladding laminated board |
CN102223758A (en) * | 2010-04-14 | 2011-10-19 | 江阴市明康绝缘玻纤有限公司 | Light-shield double-faced copper-clad laminate with phenolic paper base |
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