TW201843223A - Prepreg and production method therefor, stacked plate, printed circuit board and semiconductor package - Google Patents

Prepreg and production method therefor, stacked plate, printed circuit board and semiconductor package Download PDF

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TW201843223A
TW201843223A TW107110924A TW107110924A TW201843223A TW 201843223 A TW201843223 A TW 201843223A TW 107110924 A TW107110924 A TW 107110924A TW 107110924 A TW107110924 A TW 107110924A TW 201843223 A TW201843223 A TW 201843223A
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prepreg
precursor
thermosetting resin
treatment
resin composition
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TWI786099B (en
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串田圭祐
垣谷稔
清水浩
白男川芳克
金子辰德
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日商日立化成股份有限公司
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    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
    • C08J5/24—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs
    • C08J5/241—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs using inorganic fibres
    • C08J5/244—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs using inorganic fibres using glass fibres
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
    • C08J5/04—Reinforcing macromolecular compounds with loose or coherent fibrous material
    • C08J5/0405—Reinforcing macromolecular compounds with loose or coherent fibrous material with inorganic fibres
    • C08J5/043—Reinforcing macromolecular compounds with loose or coherent fibrous material with inorganic fibres with glass fibres
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
    • C08J5/24—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs
    • C08J5/249—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs characterised by the additives used in the prepolymer mixture
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K7/00—Use of ingredients characterised by shape
    • C08K7/02—Fibres or whiskers
    • C08K7/04—Fibres or whiskers inorganic
    • C08K7/14—Glass
    • 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
    • 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
    • H05K3/00—Apparatus or processes for manufacturing printed circuits
    • H05K3/46—Manufacturing multilayer circuits
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2300/00—Characterised by the use of unspecified polymers
    • C08J2300/24—Thermosetting resins

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Inorganic Chemistry (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Reinforced Plastic Materials (AREA)
  • Laminated Bodies (AREA)
  • Production Of Multi-Layered Print Wiring Board (AREA)

Abstract

This prepreg is obtained through the following steps 1 to 3. Step 1: a step wherein a prepreg precursor is obtained, the prepreg precursor comprising a thermosetting resin composition that has been transformed into a B-stage product, the transformation into the B-stage product comprising impregnating a substrate with the thermosetting resin composition, then performing a heat treatment thereon. Step 2: a step wherein the prepreg precursor obtained in step 1 is cooled. Step 3: a step wherein the prepreg is obtained, the prepreg being obtained by subjecting the prepreg precursor cooled in step 2 to a surface heat treatment, the surface heat treatment being a treatment that causes the surface temperature of the prepreg precursor to rise.

Description

預浸體及其製造方法、積層板、印刷線路板以及半導體封裝體Prepreg and manufacturing method thereof, laminated board, printed wiring board and semiconductor package

本發明有關一種預浸體及其製造方法、積層板、印刷線路板以及半導體封裝體。The invention relates to a prepreg and a manufacturing method thereof, a laminated board, a printed wiring board, and a semiconductor package.

近年來，電子機器的小型化、輕量化、多功能化等更加進展，伴隨此情形，大型積體電路(LSI)、晶片零件等進行高積體化，且其形態亦正朝向多接腳化及小型化急速變化。因此，為了提高電子零件的構裝密度，多層印刷線路板的微細線路化的開發持續進展。作為符合此等要求的多層印刷線路板的製造手法，例如增建方式的多層印刷線路板正逐漸作為適合輕量化、小型化及微細線路化的手法成為主流，該增建方式是使用預浸體等來作為絕緣層並一面僅以需要的部分來連接一面形成線路層，該需要的部分例如為藉由照射雷射來形成的通孔(以下亦稱為「雷射通孔」)。In recent years, miniaturization, weight reduction, and multifunctionalization of electronic devices have progressed. With this situation, large-scale integrated circuits (LSI), chip parts, and the like have been increasingly integrated, and their forms are also becoming multi-pin. And rapid changes in miniaturization. Therefore, in order to increase the mounting density of electronic parts, the development of fine wiring of multilayer printed wiring boards has continued to progress. As a manufacturing method of a multilayer printed wiring board that meets these requirements, for example, a multi-layer printed wiring board of an extension method is gradually becoming mainstream as a method suitable for weight reduction, miniaturization, and micro-wiring. The expansion method is to use a prepreg. The circuit layer is formed by waiting as an insulating layer and connecting only a required portion. The required portion is, for example, a via hole (hereinafter also referred to as a “laser via hole”) formed by irradiating a laser.

多層印刷線路板的重點在於具備：經以微細的線路間距來形成的複數層的線路圖案之間的高電性連接可靠性及優異的高頻特性，並且，要求與半導體晶片之間的連接可靠性高。特別是，近年來，在多功能型行動電話終端等的主機板中顯著進行薄型化及線路的高密度化，而正在對用以提供其層間連接的雷射通孔謀求小直徑化。 　　當以小直徑的雷射通孔來進行層間連接時，重要的特性之一可舉例如基板的尺寸安定性。在進行多層線路化時，會對各基板施行複數次加熱及複數次積層時的壓力。因此，當基板本身的尺寸偏差、特別是由熱履歷等所造成的各基板的尺寸變化量的偏差較大時，每次積層皆會發生雷射通孔的位置偏移，而可能會成為連接可靠性降低等不良情形的原因。因此，正在謀求尺寸變化量的偏差較小的基板。The important point of a multilayer printed wiring board is to have high electrical connection reliability and excellent high-frequency characteristics between a plurality of layers of circuit patterns formed at a fine line pitch, and reliable connection to a semiconductor wafer is required. High sex. In particular, in recent years, motherboards such as multifunctional mobile phone terminals have been significantly reduced in thickness and high-density lines, and laser vias for providing interlayer connections have been reduced in diameter. When interlayer connection is performed with a laser via having a small diameter, one of the important characteristics may be, for example, the dimensional stability of a substrate. When multi-layer wiring is performed, each substrate is subjected to a plurality of times of heating and a pressure during lamination. Therefore, when the dimensional deviation of the substrate itself, especially the variation in the dimensional change amount of each substrate caused by thermal history, etc., is large, the position of the laser through hole will shift every time the layer is laminated, and it may become a connection Causes of bad situations such as reduced reliability. Therefore, substrates with small variations in the amount of dimensional change are being sought.

例如：專利文獻1中，為了提高多層印刷線路板中的層間的合致性的目的，而揭示一種預浸體，其特徵在於是由下述所構成：芯部，其由基材所構成，該基材包含已預先硬化的熱硬化性樹脂且具有第1面和第2面；以及，第1黏著劑層與第2黏著劑層，該等分別形成於該芯部的第1面與第2面。 [先前技術文獻] (專利文獻)For example, Patent Document 1 discloses a prepreg for the purpose of improving the consistency between layers in a multilayer printed wiring board, which is characterized by being composed of a core portion composed of a base material, and The substrate includes a pre-cured thermosetting resin and has a first surface and a second surface; and a first adhesive layer and a second adhesive layer, which are formed on the first surface and the second surface of the core, respectively. surface. [Prior Art Literature] (Patent Literature)

專利文獻1：日本特開2002-103494號公報Patent Document 1: Japanese Patent Application Laid-Open No. 2002-103494

[發明所欲解決的問題] 　　然而，專利文獻1的預浸體，由於包含已預先硬化的熱硬化性樹脂來作為芯部，故有線路填埋性等不良這樣的問題。此外，專利文獻1的預浸體因需要硬化度不同的複數層，因此，需要繁雜的生產步驟，而正在期望一種尺寸變化量的偏差較小的預浸體，其能夠以更簡便的方法來獲得。[Problems to be Solved by the Invention] However, since the prepreg of Patent Document 1 contains a thermosetting resin that has been hardened in advance as a core portion, there is a problem such as poor line fillability. In addition, since the prepreg of Patent Document 1 requires a plurality of layers having different hardening degrees, complicated production steps are required, and a prepreg having a small variation in the dimensional change amount is expected, which can be obtained in a simpler way. obtain.

於是，本發明的目的在於提供一種預浸體及其製造方法、積層板、印刷線路板以及半導體封裝體，該預浸體的成形性優異且尺寸變化量的偏差較小。 [解決問題的技術手段]Therefore, an object of the present invention is to provide a prepreg and a method for manufacturing the same, a laminated board, a printed wiring board, and a semiconductor package, which are excellent in formability and have small variations in dimensional change. [Technical means to solve the problem]

本發明人為了達成前述目的而致力進行研究後，結果發現一種預浸體，其成形性優異且尺寸變化量的偏差較小，遂完成本發明，該預浸體是經過實施特定加熱處理的步驟來製造。本發明有關下述[1]～[10]的技術。 [1]一種預浸體，其經過下述步驟1～3來獲得： 　　步驟1：獲得預浸體前驅物的步驟，並且，前述預浸體前驅物是對熱硬化性樹脂組成物進行B階段化而成，且於前述B階段化中，使熱硬化性樹脂組成物含浸於基材中之後實施加熱處理； 　　步驟2：將步驟1中獲得的預浸體前驅物冷卻的步驟； 　　步驟3：獲得預浸體的步驟，並且，前述預浸體是對在步驟2中冷卻後的預浸體前驅物實施表面加熱處理來獲得，且前述表面加熱處理是使預浸體前驅物的表面溫度上升的處理。 [2]如上述[1]所述之預浸體，其中，步驟3中的表面加熱處理是使前述預浸體前驅物的表面溫度上升5～110℃的處理。 [3]如上述[1]或[2]所述之預浸體，其中，步驟3中的表面加熱處理是將前述預浸體前驅物的表面溫度加熱至20～130℃的處理。 [4]如上述[1]至[3]中任一項所述之預浸體，其中，步驟3中的表面加熱處理是在200～700℃的環境中將前述預浸體前驅物加熱的處理。 [5]如上述[1]至[4]中任一項所述之預浸體，其中，步驟3中的表面加熱處理的加熱時間為1.0～10.0秒。 [6]如上述[1]至[5]中任一項所述之預浸體，其中，前述基材為玻璃布。 [7]一種積層板，其是將上述[1]至[6]中任一項所述之預浸體與金屬箔積層並進行成形而成。 [8]一種印刷線路板，其是包含上述[1]至[6]中任一項所述之預浸體或上述[7]所述之積層板而成。 [9]一種半導體封裝體，其是使用上述[8]所述之印刷線路板而成。 [10]一種預浸體的製造方法，其是用以製造上述[1]至[6]中任一項所述之預浸體的方法，並且，具有下述步驟1～3： 　　步驟1：獲得預浸體前驅物的步驟，並且，前述預浸體前驅物是對熱硬化性樹脂組成物進行B階段化而成，且於前述B階段化中，使熱硬化性樹脂組成物含浸於基材中之後實施加熱處理； 　　步驟2：將步驟1中獲得的預浸體前驅物冷卻的步驟； 　　步驟3：獲得預浸體的步驟，並且，前述預浸體是對在步驟2中冷卻後的預浸體前驅物實施表面加熱處理來獲得，且前述表面加熱處理是使預浸體前驅物的表面溫度上升的處理。 [功效]The present inventors have devoted themselves to research in order to achieve the foregoing object, and as a result, have found a prepreg with excellent formability and small variation in dimensional change, and thus completed the present invention. The prepreg is a step of performing a specific heat treatment To make. The present invention relates to the following techniques [1] to [10]. [1] A prepreg obtained by the following steps 1-3: Step 1: a step of obtaining a prepreg precursor, and the prepreg precursor is a B-stage of a thermosetting resin composition It is converted into a material, and in the aforementioned B-stage conversion, the thermosetting resin composition is impregnated in the substrate and then subjected to a heat treatment; Step 2: a step of cooling the prepreg precursor obtained in Step 1; Step 3: A step of obtaining a prepreg, and the prepreg is obtained by performing a surface heating treatment on the prepreg precursor cooled in step 2, and the surface heating treatment is to increase a surface temperature of the prepreg precursor Processing. [2] The prepreg according to the above [1], wherein the surface heating treatment in step 3 is a treatment for increasing the surface temperature of the prepreg precursor by 5 to 110 ° C. [3] The prepreg according to the above [1] or [2], wherein the surface heating treatment in step 3 is a treatment of heating the surface temperature of the precursor of the prepreg to 20 to 130 ° C. [4] The prepreg according to any one of the above [1] to [3], wherein the surface heating treatment in step 3 is performed by heating the prepreg precursor in an environment of 200 to 700 ° C. deal with. [5] The prepreg according to any one of the above [1] to [4], wherein a heating time of the surface heating treatment in step 3 is 1.0 to 10.0 seconds. [6] The prepreg according to any one of the above [1] to [5], wherein the substrate is glass cloth. [7] A laminated board obtained by laminating and forming a prepreg and a metal foil according to any one of the above [1] to [6]. [8] A printed wiring board comprising the prepreg according to any one of the above [1] to [6] or the laminated board according to the above [7]. [9] A semiconductor package using the printed wiring board described in [8] above. [10] A method for producing a prepreg, which is a method for producing the prepreg according to any one of the above [1] to [6], and further includes the following steps 1 to 3: (1) Step 1: A step of obtaining a prepreg precursor, wherein the prepreg precursor is obtained by subjecting the thermosetting resin composition to B-stage, and in the B-stage forming, the thermosetting resin composition is impregnated with a base The material is then subjected to a heat treatment; Step 2: a step of cooling the prepreg precursor obtained in step 1; Step 3: a step of obtaining a prepreg, and the aforementioned prepreg is obtained after cooling in step 2 The prepreg precursor is obtained by performing a surface heating treatment, and the surface heating treatment is a treatment for increasing the surface temperature of the prepreg precursor. [efficacy]

根據本發明，能夠提供一種預浸體及其製造方法、積層板、印刷線路板以及半導體封裝體，該預浸體的成形性優異且尺寸變化量的偏差較小。According to the present invention, it is possible to provide a prepreg and a method for manufacturing the same, a laminated board, a printed wiring board, and a semiconductor package. The prepreg is excellent in formability and has a small variation in a dimensional change amount.

本說明書中，數值範圍的下限值及上限值分別能夠與其它數值範圍的下限值及上限值任意組合。本發明中亦包含將本說明書中的記載事項任意組合而成的態樣。In this specification, the lower limit value and the upper limit value of the numerical range can be arbitrarily combined with the lower limit value and the upper limit value of other numerical ranges, respectively. The present invention also includes an aspect in which the matters described in this specification are arbitrarily combined.

[預浸體] 　　本發明的預浸體是經過下述步驟1～3來獲得： 　　步驟1：獲得預浸體前驅物的步驟，並且，前述預浸體前驅物是對熱硬化性樹脂組成物進行B階段化而成，且於前述B階段化中，使熱硬化性樹脂組成物含浸於基材中之後實施加熱處理； 　　步驟2：將步驟1中獲得的預浸體前驅物冷卻的步驟； 　　步驟3：獲得預浸體的步驟，並且，前述預浸體是對在步驟2中冷卻後的預浸體前驅物實施表面加熱處理來獲得，且前述表面加熱處理是使預浸體前驅物的表面溫度上升的處理。 　　首先，說明本發明的預浸體中所使用的基材及熱硬化性樹脂組成物，然後，說明本發明的預浸體的製造方法。 　　再者，本發明中，所謂B階段，是指使熱硬化性樹脂組成物半硬化後的狀態。[Prepreg] The prepreg of the present invention is obtained through the following steps 1-3: Step 1: A step of obtaining a prepreg precursor, and the prepreg precursor is a thermosetting resin composition B-staged, and in the aforementioned B-staged, the thermosetting resin composition is impregnated in the substrate and then subjected to a heat treatment; step 2: a step of cooling the prepreg precursor obtained in step 1; Step 3: A step of obtaining a prepreg, and the prepreg is obtained by subjecting the prepreg precursor cooled in step 2 to a surface heating treatment, and the surface heating treatment is performed on the prepreg precursor. Surface temperature rise treatment. (1) First, a base material and a thermosetting resin composition used in the prepreg of the present invention will be described, and then a method for producing the prepreg of the present invention will be described. Furthermore, in the present invention, the "B-stage" means a state after the thermosetting resin composition is semi-cured.

＜基材＞ 　　本發明的預浸體所包含的基材，能夠使用例如：各種電絕緣材料用積層板中所使用的習知基材，並無特別限定。 　　作為基材，可舉例如：紙、棉絨等天然纖維；玻璃纖維、石綿等無機纖維；芳醯胺、聚醯亞胺、聚乙烯醇、聚酯、四氟乙烯、壓克力等有機纖維；此等的混合物等。此等之中，以玻璃纖維為佳。玻璃纖維基材以玻璃織布(玻璃布)為佳，可舉例如：使用E玻璃、C玻璃、D玻璃、S玻璃等而得的織布、或以有機黏合劑來將短纖維黏著而成的玻璃織布；將玻璃纖維與纖維素纖維混抄而成的基材等。較佳是使用E玻璃而得的玻璃織布。 　　此等基材具有織布、不織布、紗束、切股氈、表面氈等形狀。再者，材質及形狀是依目標的成形物的用途及性能來選擇，可單獨使用1種，且亦能夠因應需要來組合2種以上的材質及形狀。 　　基材的厚度例如為0.01～0.5 mm，從成形性及能夠高密度佈線的觀點來看，以0.015～0.2 mm為佳，以0.02～0.1 mm較佳。從耐熱性、耐濕性、加工性等觀點來看，此等基材較佳為：經以矽烷耦合劑等來進行表面處理後的基材、經實施機械性的開纖處理後的基材。<Substrate> 的 The substrate included in the prepreg of the present invention can be, for example, a conventional substrate used in a laminated board for various electrical insulating materials, and is not particularly limited. Examples of the base material include natural fibers such as paper and cotton wool; inorganic fibers such as glass fiber and asbestos; organic fibers such as aramide, polyimide, polyvinyl alcohol, polyester, tetrafluoroethylene, and acrylic ; These mixtures and so on. Among these, glass fiber is preferred. The glass fiber substrate is preferably a glass woven cloth (glass cloth). For example, a woven cloth obtained by using E glass, C glass, D glass, S glass, etc., or an organic binder is used to adhere short fibers. Glass woven fabrics; substrates made by mixing glass fibers with cellulose fibers. A glass cloth obtained by using E glass is preferred.基材 These substrates have shapes such as woven fabrics, non-woven fabrics, yarn bundles, cut strand felts, and surface felts. In addition, the material and shape are selected according to the intended use and performance of the molded product, and one type may be used alone, and two or more types of materials and shapes may be combined as required.厚度 The thickness of the base material is, for example, 0.01 to 0.5 mm. From the viewpoint of moldability and high-density wiring, it is preferably 0.015 to 0.2 mm, and more preferably 0.02 to 0.1 mm. From the viewpoints of heat resistance, moisture resistance, processability, etc., these substrates are preferably: a substrate subjected to a surface treatment with a silane coupling agent or the like, and a substrate subjected to a mechanical fiber opening treatment .

＜熱硬化性樹脂組成物＞ 　　本發明的預浸體所包含的熱硬化性樹脂組成物，能夠使用例如一種熱硬化性樹脂組成物，其含有印刷線路板用的預浸體中所使用的習知熱硬化性樹脂，並無特別限定。 　　熱硬化性樹脂組成物含有(A)熱硬化性樹脂，且較佳是進一步含有從由(B)硬化劑、(C)硬化促進劑及(D)無機填充材料所組成之群組中選出的1種以上，更佳是含有(B)硬化劑、(C)硬化促進劑及(D)無機填充材料。 　　以下，說明熱硬化性樹脂組成物能夠含有的各成分。<Thermosetting resin composition> The thermosetting resin composition included in the prepreg of the present invention can be, for example, a thermosetting resin composition containing a conventional prepreg used in a printed wiring board. The thermosetting resin is not particularly limited. The thermosetting resin composition contains (A) a thermosetting resin, and preferably further contains a member selected from the group consisting of (B) a curing agent, (C) a curing accelerator, and (D) an inorganic filler. One or more types, more preferably (B) a hardener, (C) a hardening accelerator, and (D) an inorganic filler. Hereinafter, each component which a thermosetting resin composition can contain is demonstrated.

((A)熱硬化性樹脂) 　　作為(A)熱硬化性樹脂，並無特別限制，能夠從以往作為熱硬化性樹脂使用的樹脂之中適當選擇使用任意樹脂。 　　作為(A)熱硬化性樹脂，可舉例如：環氧樹脂、酚樹脂、馬來醯亞胺化合物、氰酸酯樹脂、異氰酸酯樹脂、苯并噁嗪(benzoxazine)樹脂、氧雜環丁烷(oxetane)樹脂、胺基樹脂、不飽和聚酯樹脂、烯丙基樹脂、雙環戊二烯樹脂、矽氧樹脂、三嗪樹脂、三聚氰胺樹脂等。此等之中，從成形性及電絕緣性的觀點來看，較佳是環氧樹脂、馬來醯亞胺化合物。 　　(A)熱硬化性樹脂可單獨使用1種，亦可併用2種以上。((A) Thermosetting resin) The (A) thermosetting resin is not particularly limited, and any resin can be appropriately selected and used from among resins conventionally used as thermosetting resins. Examples of the (A) thermosetting resin include epoxy resin, phenol resin, maleimide compound, cyanate resin, isocyanate resin, benzoxazine resin, and oxetane ( oxetane) resin, amine resin, unsaturated polyester resin, allyl resin, dicyclopentadiene resin, silicone resin, triazine resin, melamine resin, and the like. Among these, an epoxy resin and a maleimide compound are preferable from a viewpoint of moldability and electrical insulation. (A) The thermosetting resin may be used singly or in combination of two or more kinds.

環氧樹脂的環氧當量以100～500 g/eq為佳，以150～400 g/eq較佳，以200～350 g/eq更佳。此處，環氧當量為每個環氧基的樹脂的質量(g/eq)，能夠依照JIS K 7236所規定的方法來進行測定。The epoxy equivalent of the epoxy resin is preferably 100 to 500 g / eq, more preferably 150 to 400 g / eq, and even more preferably 200 to 350 g / eq. Here, the epoxy equivalent is the mass (g / eq) of the resin per epoxy group, and can be measured according to the method prescribed by JIS K 7236.

作為環氧樹脂，可舉例如：縮水甘油基醚型的環氧樹脂、縮水甘油基胺型的環氧樹脂、縮水甘油酯型的環氧樹脂等。此等之中，以縮水甘油基醚型的環氧樹脂為佳。 　　環氧樹脂亦能夠依主骨架不同來分類為各種環氧樹脂，上述各型的環氧樹脂中，分別能夠進一步分類為：雙酚A型環氧樹脂、雙酚F型環氧樹脂、雙酚S型環氧樹脂等雙酚型環氧樹脂；聯苯芳烷基酚醛清漆型環氧樹脂、苯酚酚醛清漆型環氧樹脂、烷基苯酚酚醛清漆型環氧樹脂、甲酚酚醛清漆型環氧樹脂、萘酚烷基苯酚共聚酚醛清漆型環氧樹脂、萘酚芳烷基甲酚共聚酚醛清漆型環氧樹脂、雙酚A酚醛清漆型環氧樹脂、雙酚F酚醛清漆型環氧樹脂等酚醛清漆型環氧樹脂；二苯乙烯型環氧樹脂；含三嗪骨架環氧樹脂；含茀骨架環氧樹脂；萘型環氧樹脂；蒽型環氧樹脂；三苯基甲烷型環氧樹脂；聯苯型環氧樹脂；二甲苯型環氧樹脂；雙環戊二烯型環氧樹脂等脂環式環氧樹脂等。 　　此等之中，從成形性及絕緣可靠性的觀點來看，以酚醛清漆型環氧樹脂為佳，以聯苯芳烷基酚清漆型環氧樹脂較佳。Examples of the epoxy resin include a glycidyl ether epoxy resin, a glycidylamine epoxy resin, and a glycidyl ester epoxy resin. Among these, a glycidyl-ether type epoxy resin is preferable. Epoxy resins can also be classified into various epoxy resins according to the main skeleton. Among the above types of epoxy resins, they can be further classified into: bisphenol A epoxy resin, bisphenol F epoxy resin, and bisphenol. S-type epoxy resin and other bisphenol epoxy resins; biphenylaralkyl novolac epoxy resin, phenol novolac epoxy resin, alkylphenol novolac epoxy resin, cresol novolac epoxy Resin, naphthol alkylphenol copolymer novolac epoxy resin, naphthol aralkyl cresol copolymer novolac epoxy resin, bisphenol A novolac epoxy resin, bisphenol F novolac epoxy resin, etc. Novolac epoxy resin; stilbene epoxy resin; triazine skeleton epoxy resin; fluorene skeleton epoxy resin; naphthalene epoxy resin; anthracene epoxy resin; triphenylmethane epoxy resin ; Biphenyl epoxy resin; xylene epoxy resin; alicyclic epoxy resin such as dicyclopentadiene epoxy resin. Among these, from the viewpoint of moldability and insulation reliability, novolac-type epoxy resins are preferred, and biphenylaralkyl novolac-type epoxy resins are preferred.

作為馬來醯亞胺化合物，較佳是具有N-取代馬來醯亞胺基之馬來醯亞胺化合物(a1)(以下，亦稱為「馬來醯亞胺化合物(a1)」)。 　　作為馬來醯亞胺化合物(a1)，具體而言，可舉例如：N,N’-伸乙基雙馬來醯亞胺、N,N’-六亞甲基雙馬來醯亞胺、雙(4-馬來醯亞胺基環己基)甲烷、1,4-雙(馬來醯亞胺基甲基)環己烷等含脂肪族烴基馬來醯亞胺；N,N’-(1,3-伸苯基)雙馬來醯亞胺、N,N’-[1,3-(2-甲基伸苯基)]雙馬來醯亞胺、N,N’-[1,3-(4-甲基伸苯基)]雙馬來醯亞胺、N,N’-(1,4-伸苯基)雙馬來醯亞胺、雙(4-馬來醯亞胺基苯基)甲烷、雙(3-甲基-4-馬來醯亞胺基苯基)甲烷、3,3’-二甲基-5,5’-二乙基-4,4’-二苯基甲烷雙馬來醯亞胺、雙(4-馬來醯亞胺基苯基)醚、雙(4-馬來醯亞胺基苯基)碸、雙(4-馬來醯亞胺基苯基)硫醚、雙(4-馬來醯亞胺基苯基)酮、1,4-雙(4-馬來醯亞胺基苯基)環己烷、1,4-雙(馬來醯亞胺基甲基)環己烷、1,3-雙(4-馬來醯亞胺基苯氧基)苯、1,3-雙(3-馬來醯亞胺基苯氧基)苯、雙[4-(3-馬來醯亞胺基苯氧基)苯基]甲烷、雙[4-(4-馬來醯亞胺基苯氧基)苯基]甲烷、1,1-雙[4-(3-馬來醯亞胺基苯氧基)苯基]乙烷、1,1-雙[4-(4-馬來醯亞胺基苯氧基)苯基]乙烷、1,2-雙[4-(3-馬來醯亞胺基苯氧基)苯基]乙烷、1,2-雙[4-(4-馬來醯亞胺基苯氧基)苯基]乙烷、2,2-雙[4-(3-馬來醯亞胺基苯氧基)苯基]丙烷、2,2-雙[4-(4-馬來醯亞胺基苯氧基)苯基]丙烷、2,2-雙[4-(3-馬來醯亞胺基苯氧基)苯基]丁烷、2,2-雙[4-(4-馬來醯亞胺基苯氧基)苯基]丁烷、2,2-雙[4-(3-馬來醯亞胺基苯氧基)苯基]-1,1,1,3,3,3-六氟丙烷、2,2-雙[4-(4-馬來醯亞胺基苯氧基)苯基]-1,1,1,3,3,3-六氟丙烷、4,4-雙(3-馬來醯亞胺基苯氧基)聯苯、4,4-雙(4-馬來醯亞胺基苯氧基)聯苯、雙[4-(3-馬來醯亞胺基苯氧基)苯基]酮、雙[4-(4-馬來醯亞胺基苯氧基)苯基]酮、2,2’-雙(4-馬來醯亞胺基苯基)二硫醚、雙(4-馬來醯亞胺基苯基)二硫醚、雙[4-(3-馬來醯亞胺基苯氧基)苯基]硫醚、雙[4-(4-馬來醯亞胺基苯氧基)苯基]硫醚、雙[4-(3-馬來醯亞胺基苯氧基)苯基]亞碸、雙[4-(4-馬來醯亞胺基苯氧基)苯基]亞碸、雙[4-(3-馬來醯亞胺基苯氧基)苯基]碸、雙[4-(4-馬來醯亞胺基苯氧基)苯基]碸、雙[4-(3-馬來醯亞胺基苯氧基)苯基]醚、雙[4-(4-馬來醯亞胺基苯氧基)苯基]醚、1,4-雙[4-(4-馬來醯亞胺基苯氧基)-α,α-二甲基苯甲基]苯、1,3-雙[4-(4-馬來醯亞胺基苯氧基)-α,α-二甲基苯甲基]苯、1,4-雙[4-(3-馬來醯亞胺基苯氧基)-α,α-二甲基苯甲基]苯、1,3-雙[4-(3-馬來醯亞胺基苯氧基)-α,α-二甲基苯甲基]苯、1,4-雙[4-(4-馬來醯亞胺基苯氧基)-3,5-二甲基-α,α-二甲基苯甲基]苯、1,3-雙[4-(4-馬來醯亞胺基苯氧基)-3,5-二甲基-α,α-二甲基苯甲基]苯、1,4-雙[4-(3-馬來醯亞胺基苯氧基)-3,5-二甲基-α,α-二甲基苯甲基]苯、1,3-雙[4-(3-馬來醯亞胺基苯氧基)-3,5-二甲基-α,α-二甲基苯甲基]苯、聚苯基甲烷馬來醯亞胺等含芳香族烴基馬來醯亞胺。 　　此等之中，從反應率高、能夠更加高耐熱性化這樣的觀點來看，較佳是雙(4-馬來醯亞胺基苯基)甲烷、雙(4-馬來醯亞胺基苯基)碸、雙(4-馬來醯亞胺基苯基)硫醚、雙(4-馬來醯亞胺基苯基)二硫醚、N,N’-(1,3-伸苯基)雙馬來醯亞胺、2,2-雙[4-(4-馬來醯亞胺基苯氧基)苯基]丙烷，從價廉這樣的觀點來看，較佳是較佳是雙(4-馬來醯亞胺基苯基)甲烷、N,N’-(1,3-伸苯基)雙馬來醯亞胺，從對溶劑的溶解性的觀點來看，特佳是雙(4-馬來醯亞胺基苯基)甲烷。The maleimide compound is preferably a maleimide compound (a1) having an N-substituted maleimide group (hereinafter, also referred to as a "maleimide compound (a1)"). Specific examples of the maleimidine imine compound (a1) include N, N'-ethylidenebismaleimide, N, N'-hexamethylenebismaleimide, Aliphatic hydrocarbon-containing maleimide, such as bis (4-maleimidoiminocyclohexyl) methane, 1,4-bis (maleimidoiminomethyl) cyclohexane; N, N '-( 1,3-phenylene) bismaleimide, N, N '-[1,3- (2-methylphenylene)] bismaleimide, N, N'-[1, 3- (4-methylphenylene)] bismaleimide, N, N '-(1,4-phenylene) bismaleimide, bis (4-maleimide) Phenyl) methane, bis (3-methyl-4-maleimidophenyl) methane, 3,3'-dimethyl-5,5'-diethyl-4,4'-diphenyl Methylmethanebismaleimide, bis (4-maleimidoiminophenyl) ether, bis (4-maleimidoiminophenyl) fluorene, bis (4-maleimidoiminophenyl) Sulfide), bis (4-maleimidoiminophenyl) ketone, 1,4-bis (4-maleimidoiminophenyl) cyclohexane, 1,4-bis (maleimido Iminomethyl) cyclohexane, 1,3-bis (4-maleimidoimidophenoxy) benzene, 1,3-bis (3-maleimidoimidophenoxy) benzene, Bis (4- (3-maleimidoiminophenoxy) Phenyl] methane, bis [4- (4-maleimidoimidophenoxy) phenyl] methane, 1,1-bis [4- (3-maleimidoimidophenoxy) phenyl ] Ethane, 1,1-bis [4- (4-maleimidoimidophenoxy) phenyl] ethane, 1,2-bis [4- (3-maleimidoimidophenoxy) Yl) phenyl] ethane, 1,2-bis [4- (4-maleimidoiminophenoxy) phenyl] ethane, 2,2-bis [4- (3-maleimidine Aminophenoxy) phenyl] propane, 2,2-bis [4- (4-maleimidoiminophenoxy) phenyl] propane, 2,2-bis [4- (3-Malay醯 iminophenoxy) phenyl] butane, 2,2-bis [4- (4-maleimidoiminophenoxy) phenyl] butane, 2,2-bis [4- ( 3-maleimidoiminophenoxy) phenyl] -1,1,1,3,3,3-hexafluoropropane, 2,2-bis [4- (4-maleimidoiminobenzene (Oxy) phenyl) -1,1,1,3,3,3-hexafluoropropane, 4,4-bis (3-maleimidophenoxy) biphenyl, 4,4-bis ( 4-maleimidophenoxy) biphenyl, bis [4- (3-maleimidophenoxy) phenyl] one, bis [4- (4-maleimidoimino Phenoxy) phenyl] ketone, 2,2'-bis (4-maleimidophenyl) disulfide, bis (4-maleimidophenyl) disulfide, bis [ 4- (3-maleimidophenoxy ) Phenyl] sulfide, bis [4- (4-maleimidophenoxy) phenyl] phenyl] sulfide, bis [4- (3-maleimidophenoxy) phenyl] Fluorene, bis [4- (4-maleimidoiminophenoxy) phenyl] fluorene, bis [4- (3-maleiminoimidophenoxy) phenyl] fluorene, bis [ 4- (4-maleimidoiminophenoxy) phenyl] fluorene, bis [4- (3-maleimidoiminophenoxy) phenyl] ether, bis [4- (4-Ma Lymeiminophenoxy) phenyl] ether, 1,4-bis [4- (4-maleimidoiminophenoxy) -α, α-dimethylbenzyl] benzene, 1 , 3-bis [4- (4-maleimidophenoxy) -α, α-dimethylbenzyl] benzene, 1,4-bis [4- (3-maleimidoimine Phenylphenoxy) -α, α-dimethylbenzyl] benzene, 1,3-bis [4- (3-maleimidoiminophenoxy) -α, α-dimethylbenzyl Phenyl] benzene, 1,4-bis [4- (4-maleimidoiminophenoxy) -3,5-dimethyl-α, α-dimethylbenzyl] benzene, 1,3 -Bis [4- (4-maleimidophenoxy) -3,5-dimethyl-α, α-dimethylbenzyl] benzene, 1,4-bis [4- (3 -Maleimidophenoxy) -3,5-dimethyl-α, α-dimethylbenzyl] benzene, 1,3-bis [4- (3-maleimidoimino (Phenoxy) -3,5-dimethyl-α, α-dimethyl Aromatic hydrocarbon-containing maleimide, such as benzyl] benzene, polyphenylmethane maleimide, and the like. Among these, bis (4-maleimidoiminophenyl) methane and bis (4-maleimidoimino) are preferred from the viewpoint of high reaction rate and higher heat resistance. Phenyl) fluorene, bis (4-maleiminoiminophenyl) sulfide, bis (4-maleiminoiminophenyl) disulfide, N, N '-(1,3-phenylene Group) bismaleimidine imine, 2,2-bis [4- (4-maleimidoiminophenoxy) phenyl] propane, from the viewpoint of low cost, preferably, more preferably From the viewpoint of solubility in a solvent, bis (4-maleimidophenyl) methane and N, N '-(1,3-phenylene) bismaleimidoimine are particularly preferred. Bis (4-maleiminophenylene) methane.

馬來醯亞胺化合物，較佳是一種具有N-取代馬來醯亞胺基之馬來醯亞胺化合物，其是使馬來醯亞胺化合物(a1)、具有酸性取代基之單胺化合物(a2)及二胺化合物(a3)進行反應來獲得。 　　作為具有酸性取代基之單胺化合物(a2)，可舉例如：鄰胺基苯酚、間胺基苯酚、對胺基苯酚、鄰胺基苯甲酸、間胺基苯甲酸、對胺基苯甲酸、鄰胺基苯磺酸、間胺基苯磺酸、對胺基苯磺酸、3,5-二羥基苯胺、3,5-二羧基苯胺等。 　　作為二胺化合物(a3)，具體而言，可舉例如：4,4’-二胺基二苯基甲烷、4,4’-二胺基二苯基乙烷、4,4’-二胺基二苯基丙烷、2,2’-雙[4,4’-二胺基二苯基]丙烷、3,3’-二甲基-4,4’-二胺基二苯基甲烷、3,3’-二乙基-4,4’-二胺基二苯基甲烷、3,3’-二甲基-4,4’-二胺基二苯基乙烷、3,3’-二乙基-4,4’-二胺基二苯基乙烷、4,4’-二胺基二苯基醚、4,4’-二胺基二苯基硫醚、3,3’-二羥基-4,4’-二胺基二苯基甲烷、2,2’,6,6’-四甲基-4,4’-二胺基二苯基甲烷、3,3’-二氯-4,4’-二胺基二苯基甲烷、3,3’-二溴-4,4’-二胺基二苯基甲烷、2,2’,6,6’-四甲基氯-4,4’-二胺基二苯基甲烷、2,2’,6,6’-四溴-4,4’-二胺基二苯基甲烷等。此等之中，從價廉這樣的觀點來看，較佳是4,4’-二胺基二苯基甲烷、3,3’-二乙基-4,4’-二胺基二苯基甲烷，從對溶劑的溶解性的觀點看，更佳是4,4’-二胺基二苯基甲烷。A maleimide compound, preferably a maleimide compound having an N-substituted maleimide group, is a maleimide compound (a1), a monoamine compound having an acidic substituent (a2) is obtained by reacting with a diamine compound (a3). Examples of the monoamine compound (a2) having an acidic substituent include o-aminophenol, m-aminophenol, p-aminophenol, o-aminobenzoic acid, m-aminobenzoic acid, p-aminobenzoic acid, O-aminobenzenesulfonic acid, m-aminobenzenesulfonic acid, p-aminobenzenesulfonic acid, 3,5-dihydroxyaniline, 3,5-dicarboxyaniline and the like. Specific examples of the diamine compound (a3) include 4,4'-diaminodiphenylmethane, 4,4'-diaminodiphenylethane, and 4,4'-diamine. Diphenylpropane, 2,2'-bis [4,4'-diaminodiphenyl] propane, 3,3'-dimethyl-4,4'-diaminodiphenylmethane, 3 , 3'-diethyl-4,4'-diaminodiphenylmethane, 3,3'-dimethyl-4,4'-diaminodiphenylethane, 3,3'-di Ethyl-4,4'-diaminodiphenylethane, 4,4'-diaminodiphenyl ether, 4,4'-diaminodiphenylsulfide, 3,3'-di Hydroxy-4,4'-diaminodiphenylmethane, 2,2 ', 6,6'-tetramethyl-4,4'-diaminodiphenylmethane, 3,3'-dichloro- 4,4'-diaminodiphenylmethane, 3,3'-dibromo-4,4'-diaminodiphenylmethane, 2,2 ', 6,6'-tetramethyl chloride-4 , 4'-diaminodiphenylmethane, 2,2 ', 6,6'-tetrabromo-4,4'-diaminodiphenylmethane and the like. Among these, 4,4'-diaminodiphenylmethane and 3,3'-diethyl-4,4'-diaminodiphenyl are preferred from the viewpoint of low cost. Methane is more preferably 4,4'-diaminodiphenylmethane from the viewpoint of solubility in a solvent.

馬來醯亞胺化合物(a1)、具有酸性取代基之單胺化合物(a2)及二胺化合物(a3)的反應中，三者的使用量較佳是：具有酸性取代基之單胺化合物(a2)與二胺化合物(a3)具有的一級胺基當量[記載為－NH2 基當量]的合計與馬來醯亞胺化合物(a1)的馬來醯亞胺基當量之間的關係，滿足下述式。 　 0.1≦[馬來醯亞胺基當量]/[－NH2 基當量的合計]≦10 　　藉由將[馬來醯亞胺基當量]/[－NH2 基當量的合計]設為0.1以上，便能夠不降低凝膠化及耐熱性，並且，藉由將[馬來醯亞胺基當量]/[－NH2 基當量的合計]設為10以下，便能夠不降低對有機溶劑的溶解性、金屬箔黏著性及耐熱性，故較佳。 　　從相同的觀點來看，更佳是滿足下述式。 1≦[馬來醯亞胺基當量]/[－NH2 基當量的合計]≦9 　　更佳是滿足下述式。 　 2≦[馬來醯亞胺基當量]/[－NH2 基當量的合計]≦8In the reaction of the maleimide compound (a1), the monoamine compound (a2) having an acidic substituent, and the diamine compound (a3), the amount of the three used is preferably: a monoamine compound having an acidic substituent ( a2) The relationship between the total of the primary amine equivalents [documented as -NH 2 group equivalents] possessed by the diamine compound (a3) and the maleimide imide equivalents of the maleimide compound (a1), satisfying The following formula. 0.1 ≦ [maleimide imide equivalent] / [-total of NH 2 radical equivalent] ≦ 10 By setting [maleimide imide equivalent] / [— NH 2 radical equivalent] to 0.1 or more, It is possible not to reduce gelation and heat resistance, and by setting [maleimide imide equivalent] / [-NH 2 group equivalent] to 10 or less, it is possible to prevent the solubility in organic solvents from being reduced. , Metal foil adhesion and heat resistance, so it is better. From the same viewpoint, it is more preferable to satisfy the following formula. 1 ≦ [maleimide imide equivalent] / [-total of NH 2 group equivalent] ≦ 9 is more preferable to satisfy the following formula. 2 ≦ [maleimide imide equivalent] / [-total of NH 2 group equivalent] ≦ 8

相對於熱硬化性樹脂組成物中的樹脂成分100質量份，熱硬化性樹脂組成物中的(A)熱硬化性樹脂的含量以15～80質量份為佳，以25～70質量份較佳，以35～60質量份更佳。所謂熱硬化性樹脂組成物中的樹脂成分，是指例如(A)熱硬化性樹脂、(B)硬化劑、(C)硬化促進劑等。The content of the (A) thermosetting resin in the thermosetting resin composition is preferably 15 to 80 parts by mass, and more preferably 25 to 70 parts by mass based on 100 parts by mass of the resin component in the thermosetting resin composition. It is more preferably 35 to 60 parts by mass. The resin component in the thermosetting resin composition refers to, for example, (A) a thermosetting resin, (B) a curing agent, (C) a curing accelerator, and the like.

((B)硬化劑) 　　為了使(A)熱硬化性樹脂硬化，熱硬化性樹脂組成物可含有(B)硬化劑。(B)硬化劑無特別限制，能夠從以往作為熱硬化性樹脂的硬化劑使用的硬化劑之中適當選擇任意硬化劑。 　　(B)硬化劑可單獨使用1種，且亦可併用2種以上。 　　當使用環氧樹脂來作為(A)熱硬化性樹脂時，作為(B)硬化劑，可舉例如：酚樹脂系硬化劑、酸酐系硬化劑、胺系硬化劑、雙氰胺、氰酸酯樹脂系硬化劑等。此等之中，從成形性及絕緣可靠性的觀點來看，以酚樹脂系硬化劑為佳。((B) Hardener) In order to harden the (A) thermosetting resin, the thermosetting resin composition may contain (B) a hardener. (B) There is no restriction | limiting in particular as a hardening | curing agent, Any hardening | curing agent can be suitably selected from the hardening | curing agents conventionally used as the hardening | curing agent of a thermosetting resin. (B) A hardener may be used individually by 1 type, and may use 2 or more types together. When an epoxy resin is used as the (A) thermosetting resin, examples of the (B) curing agent include a phenol resin-based curing agent, an acid anhydride-based curing agent, an amine-based curing agent, dicyandiamide, and cyanate ester. Resin-based hardener. Among these, from the viewpoint of moldability and insulation reliability, a phenol resin-based hardener is preferred.

作為酚樹脂系硬化劑，只要為1分子中具有2個以上的酚性羥基之酚樹脂，則無特別限制，可舉例如：間苯二酚、兒茶酚、雙酚A、雙酚F、聯苯酚等1分子中具有2個以上的酚性羥基之化合物；芳烷基型酚樹脂；雙環戊二烯型酚樹脂；三苯基甲烷型酚樹脂；苯酚酚醛清漆樹脂、甲酚酚醛清漆樹脂、胺基三嗪改質酚醛清漆型酚樹脂等酚醛清漆型酚樹脂；甲階(resol)型酚樹脂；苯甲醛型酚與芳烷基型酚的共聚型酚樹脂；對二甲苯及/或間二甲苯改質酚樹脂；三聚氰胺改質酚樹脂；萜烯改質酚樹脂；雙環戊二烯型萘酚樹脂；環戊二烯改質酚樹脂；多環芳香環改質酚樹脂；聯苯型酚樹脂等。此等之中，以酚醛清漆型酚樹脂為佳，以甲酚酚醛清漆樹脂較佳。The phenol resin-based hardener is not particularly limited as long as it is a phenol resin having two or more phenolic hydroxyl groups in one molecule, and examples thereof include resorcinol, catechol, bisphenol A, bisphenol F, Compounds having two or more phenolic hydroxyl groups in one molecule such as biphenol; aralkyl-type phenol resin; dicyclopentadiene-type phenol resin; triphenylmethane-type phenol resin; phenol novolac resin, cresol novolac resin Novolac-type phenol resins such as aminotriazine modified novolac-type phenol resins; resol-type phenol resins; copolymerized phenol resins of benzaldehyde-type phenols and aralkyl-type phenols; p-xylene and / or M-xylene modified phenol resin; melamine modified phenol resin; terpene modified phenol resin; dicyclopentadiene-type naphthol resin; cyclopentadiene modified phenol resin; polycyclic aromatic ring modified phenol resin; biphenyl Type phenol resin and so on. Among these, a novolac type phenol resin is preferable, and a cresol novolac resin is more preferable.

作為酸酐系硬化劑，可舉例如：鄰苯二甲酸酐、3-甲基-1,2,3,6-四氫鄰苯二甲酸酐、4-甲基-1,2,3,6-四氫鄰苯二甲酸酐、3-甲基六氫鄰苯二甲酸酐、4-甲基六氫鄰苯二甲酸酐、甲基-3,6-內亞甲基-1,2,3,6-四氫鄰苯二甲酸酐、二苯甲酮四甲酸二酐、甲基納迪克酸等。 　　作為胺系硬化劑，可舉例如：二伸乙三胺、三伸乙四胺、二乙胺基丙胺等鏈狀脂肪族多胺；N-胺基乙基哌嗪、異佛酮二胺等環狀脂肪族多胺；間苯二甲胺等具有芳香環的脂肪族二胺；間苯二胺、二胺基二苯基甲烷、二胺基二苯基碸等芳香族胺；胍脲等。 　　作為氰酸酯樹脂系硬化劑，可舉例如：2,2-雙(4-氰酸基苯基)丙烷、雙(4-氰酸基苯基)乙烷、雙(3,5-二甲基-4-氰酸基苯基)甲烷、2,2-雙(4-氰酸基苯基)-1,1,1,3,3,3-六氟丙烷、α,α’-雙(4-氰酸基苯基)間二異丙基苯、苯酚加成雙環戊二烯聚合物的氰酸酯化合物、苯酚酚醛清漆型氰酸酯化合物、甲酚酚醛清漆型氰酸酯化合物等。Examples of the acid anhydride-based hardener include phthalic anhydride, 3-methyl-1,2,3,6-tetrahydrophthalic anhydride, and 4-methyl-1,2,3,6- Tetrahydrophthalic anhydride, 3-methylhexahydrophthalic anhydride, 4-methylhexahydrophthalic anhydride, methyl-3,6-endemethylene-1,2,3, 6-tetrahydrophthalic anhydride, benzophenonetetracarboxylic dianhydride, methylnadic acid, etc. Examples of the amine-based hardener include: chain aliphatic polyamines such as ethylene glycol triamine, ethylene glycol tetramine, and diethylaminopropylamine; N-aminoethylpiperazine, isophorone diamine, and the like Cyclic aliphatic polyamines; aliphatic diamines with aromatic rings such as m-xylylenediamine; aromatic amines such as m-xylylenediamine, diaminodiphenylmethane, and diaminodiphenylphosphonium; guanyl urea . Examples of the cyanate resin-based hardener include 2,2-bis (4-cyanophenyl) propane, bis (4-cyanophenyl) ethane, and bis (3,5-dimethyl) Methyl-4-cyanophenyl) methane, 2,2-bis (4-cyanophenyl) -1,1,1,3,3,3-hexafluoropropane, α, α'-bis ( 4-cyanophenyl) m-isopropylbenzene, cyanate compounds of phenol-added dicyclopentadiene polymers, phenol novolac type cyanate compounds, cresol novolac type cyanate compounds, and the like.

當熱硬化性樹脂組成物含有(B)硬化劑時，相對於熱硬化性樹脂組成物中的樹脂成分100質量份，(B)硬化劑的含量以15～80質量份為佳，以25～70質量份較佳，以35～60質量份更佳。When the thermosetting resin composition contains (B) a curing agent, the content of (B) the curing agent is preferably 15 to 80 parts by mass, and 25 to 25 parts by mass based on 100 parts by mass of the resin component in the thermosetting resin composition. 70 parts by mass is preferable, and 35 to 60 parts by mass is more preferable.

當使用環氧樹脂來作為(A)熱硬化性樹脂時，源自環氧樹脂的環氧基與源自(B)硬化劑的活性氫相對於環氧基的當量比(活性氫/環氧基)以0.5～3為佳，以0.7～2.5較佳，以0.8～2.2更佳。When an epoxy resin is used as the (A) thermosetting resin, the equivalent ratio of the epoxy group derived from the epoxy resin to the active hydrogen derived from the (B) hardener relative to the epoxy group (active hydrogen / epoxy It is preferably 0.5 to 3, more preferably 0.7 to 2.5, and still more preferably 0.8 to 2.2.

((C)硬化促進劑) 　　作為(C)硬化促進劑並無特別限制，能夠從以往作為熱硬化性樹脂的硬化促進劑使用的硬化促進劑之中適當選擇任意硬化促進劑。 　　(C)硬化促進劑可單獨使用1種，且亦可併用2種以上。 　　作為(C)硬化促進劑，可舉例如：磷系化合物；咪唑化合物及其衍生物；三級胺化合物；四級銨化合物等。此等之中，從促進硬化反應的觀點來看，以咪唑化合物及其衍生物為佳。((C) Hardening Accelerator) The hardening accelerator (C) is not particularly limited, and any hardening accelerator can be appropriately selected from among hardening accelerators conventionally used as hardening accelerators for thermosetting resins. (C) A hardening accelerator may be used individually by 1 type, and may use 2 or more types together. As the hardening accelerator (C), for example, phosphorus compounds; imidazole compounds and derivatives thereof; tertiary amine compounds; quaternary ammonium compounds and the like. Among these, from the viewpoint of accelerating the hardening reaction, an imidazole compound and a derivative thereof are preferable.

作為咪唑化合物及其衍生物，可舉例如：2-甲基咪唑、2-乙基咪唑、2-十一烷基咪唑、2-十七烷基咪唑、2-苯基咪唑、1,2-二甲基咪唑、2-乙基-1-甲基咪唑、1,2-二乙基咪唑、1-乙基-2-甲基咪唑、2-乙基-4-甲基咪唑、4-乙基-2-甲基咪唑、2-苯基-4-甲基咪唑、1-苯甲基-2-苯基咪唑、1-氰乙基-2-甲基咪唑、1-氰乙基-2-乙基咪唑、1-氰乙基-2-苯基咪唑、1-氰乙基-2-乙基-4-甲基咪唑、2-苯基-4,5-二羥甲基咪唑、2-苯基-4-甲基-5-羥甲基咪唑、2,3-二氫-1H-吡咯并[1,2-a]苯并咪唑、2,4-二胺基-6-[2’-甲基咪唑基-(1’)]乙基-s-三嗪、2,4-二胺基-6-[2’-十一烷基咪唑基-(1’)]乙基-s-三嗪、2,4-二胺基-6-[2’-乙基-4’-甲基咪唑基-(1’)]乙基-s-三嗪等咪唑化合物；前述咪唑化合物與偏苯三甲酸的加成反應物；前述咪唑化合物與異氰脲酸的加成反應物；前述咪唑化合物與氫溴酸的加成反應物；前述咪唑化合物與環氧樹脂的加成反應物等。Examples of the imidazole compound and its derivative include 2-methylimidazole, 2-ethylimidazole, 2-undecylimidazole, 2-heptadecylimidazole, 2-phenylimidazole, 1,2- Dimethylimidazole, 2-ethyl-1-methylimidazole, 1,2-diethylimidazole, 1-ethyl-2-methylimidazole, 2-ethyl-4-methylimidazole, 4-ethyl 2-methylimidazole, 2-phenyl-4-methylimidazole, 1-benzyl-2-phenylimidazole, 1-cyanoethyl-2-methylimidazole, 1-cyanoethyl-2 -Ethylimidazole, 1-cyanoethyl-2-phenylimidazole, 1-cyanoethyl-2-ethyl-4-methylimidazole, 2-phenyl-4,5-dihydroxymethylimidazole, 2 -Phenyl-4-methyl-5-hydroxymethylimidazole, 2,3-dihydro-1H-pyrrolo [1,2-a] benzimidazole, 2,4-diamino-6- [2 '-Methylimidazolyl- (1')] ethyl-s-triazine, 2,4-diamino-6- [2'-undecylimidazolyl- (1 ')] ethyl-s -Triazine, 2,4-diamino-6- [2'-ethyl-4'-methylimidazolyl- (1 ')] ethyl-s-triazine; and other imidazole compounds; Addition reaction product of trimellitic acid; addition reaction product of the aforementioned imidazole compound and isocyanuric acid; addition reaction product of the aforementioned imidazole compound and hydrobromic acid; Azole compound and an addition reaction product of an epoxy resin and the like.

當熱硬化性樹脂組成物含有(C)硬化促進劑時，相對於熱硬化性樹脂組成物中的樹脂成分100質量份，(C)硬化促進劑的含量以0.01～2質量份為佳，以0.02～1.5質量份較佳，以0.04～1質量份更佳。When the thermosetting resin composition contains (C) a curing accelerator, the content of the (C) curing accelerator is preferably 0.01 to 2 parts by mass based on 100 parts by mass of the resin component in the thermosetting resin composition. 0.02 to 1.5 parts by mass is preferable, and 0.04 to 1 part by mass is more preferable.

((D)無機填充材料) 　　從低熱膨脹性等觀點來看，熱硬化性樹脂組成物可進一步含有(D)無機填充材料。 　　作為(D)無機填充材料並無特別限制，能夠從以往作為熱硬化性樹脂的無機填充材料使用的無機填充材料之中適當選擇任意無機填充材料。 　　(D)無機填充材料可單獨使用1種，且亦可併用2種以上。 　　作為(D)無機填充材料，可舉例如：氧化矽、氧化鋁、硫酸鋇、滑石、雲母、高嶺土、水鋁石、氧化鈹、鈦酸鋇、鈦酸鉀、鈦酸鍶、鈦酸鈣、碳酸鋁、氫氧化鎂、氫氧化鋁、硼酸鋁、矽酸鋁、碳酸鈣、矽酸鈣、矽酸鎂、硼酸鋅、錫酸鋅、氧化鋅、氧化鈦、碳化矽、氮化矽、氮化硼、煅燒黏土等黏土、玻璃短纖維、玻璃粉、中空玻璃珠等。玻璃可舉例如：E玻璃、T玻璃、D玻璃等。此等之中，從低熱膨脹性的觀點來看，以氧化矽為佳。 　　作為氧化矽，可舉例如：以濕式法來製造而含水率高的沉積氧化矽；及，以乾式法來製造而幾乎不含鍵結水等的乾式法氧化矽。作為乾式法氧化矽，可進一步依製造法不同來舉例如：粉碎氧化矽、發煙氧化矽、熔融氧化矽(熔融球狀氧化矽)等。此等之中，從低熱膨脹性及填充在樹脂中時的高流動性的觀點來看，以熔融氧化矽為佳。((D) Inorganic Filler) From the viewpoint of low thermal expansion and the like, the thermosetting resin composition may further contain (D) an inorganic filler. As the (D) inorganic filler, there is no particular limitation, and any inorganic filler can be appropriately selected from inorganic fillers conventionally used as inorganic fillers for thermosetting resins. The) (D) inorganic filler can be used singly or in combination of two or more kinds. Examples of the (D) inorganic filler include silica, alumina, barium sulfate, talc, mica, kaolin, gibbsite, beryllia, barium titanate, potassium titanate, strontium titanate, calcium titanate, Aluminum carbonate, magnesium hydroxide, aluminum hydroxide, aluminum borate, aluminum silicate, calcium carbonate, calcium silicate, magnesium silicate, zinc borate, zinc stannate, zinc oxide, titanium oxide, silicon carbide, silicon nitride, nitrogen Boron, calcined clay and other clays, short glass fibers, glass powder, hollow glass beads, etc. Examples of the glass include E glass, T glass, and D glass. Among these, silicon oxide is preferred from the viewpoint of low thermal expansion. (2) As the silicon oxide, for example, a deposited silicon oxide produced by a wet method and having a high water content; and a dry silicon oxide produced by a dry method with almost no bonding water or the like. The dry-type silicon oxide can be further classified according to different manufacturing methods, such as pulverized silicon oxide, fumed silicon oxide, fused silica (fused spherical silica), and the like. Among these, fused silica is preferable from the viewpoints of low thermal expansion and high fluidity when filled in a resin.

氧化矽，較佳是經藉由矽烷耦合劑來進行表面處理後的氧化矽。 　　作為矽烷耦合劑，可舉例如：胺基矽烷系耦合劑、環氧基矽烷系耦合劑、苯基矽烷系耦合劑、烷基矽烷系耦合劑、烯基矽烷系耦合劑、炔基矽烷系耦合劑、鹵烷基矽烷系耦合劑、矽氧烷系耦合劑、氫矽烷系耦合劑、矽氮烷系耦合劑、烷氧基矽烷系耦合劑、氯矽烷系耦合劑、(甲基)丙烯酸系矽烷系耦合劑、胺基矽烷系耦合劑、異氰脲酸基矽烷系耦合劑、脲基矽烷系耦合劑、巰基矽烷系耦合劑、硫醚矽烷系耦合劑、異氰酸基矽烷系耦合劑等。The silicon oxide is preferably silicon oxide subjected to a surface treatment with a silane coupling agent. Examples of the silane coupling agent include an aminosilane-based coupling agent, an epoxysilane-based coupling agent, a phenylsilane-based coupling agent, an alkylsilane-based coupling agent, an alkenylsilane-based coupling agent, and an alkynylsilane-based coupling agent. Agent, haloalkylsilane-based coupling agent, silicone-based coupling agent, hydrosilane-based coupling agent, silazane-based coupling agent, alkoxysilane-based coupling agent, chlorosilane-based coupling agent, (meth) acrylic Silane-based coupling agent, amine-based silane-based coupling agent, isocyanurate-based silane-based coupling agent, urea-based silane-based coupling agent, mercaptosilane-based coupling agent, thioether silane-based coupling agent, isocyanate-based silane coupling agent Wait.

(D)無機填充材料的平均粒徑以0.01～6 μm為佳，以0.1～5 μm較佳，以0.5～4 μm更佳，以1～3 μm特佳。 　　再者，本說明書中，所謂平均粒徑，是指將粒子的總體積設為100％並藉由粒徑來求出累積粒度分布曲線時相當於體積50％的點的粒徑，能夠以使用雷射繞射散射法的粒度分布測定裝置等來進行測定。(D) The average particle diameter of the inorganic filler is preferably 0.01 to 6 μm, more preferably 0.1 to 5 μm, more preferably 0.5 to 4 μm, and particularly preferably 1 to 3 μm. In addition, in this specification, the average particle diameter refers to the particle diameter of a point corresponding to 50% of the volume when the total particle size distribution curve is set to 100% of the total volume of the particles, and can be used as The measurement is performed by a particle size distribution measuring device such as a laser diffraction scattering method.

當熱硬化性樹脂組成物含有(D)無機填充材料時，從低熱膨脹性及成形性的觀點來看，相對於熱硬化性樹脂組成物中的樹脂成分100質量份，(D)無機填充材料的含量以10～300質量份為佳，以50～250質量份較佳，以100～220質量份更佳，以130～200質量份特佳。When the thermosetting resin composition contains (D) an inorganic filler, (D) an inorganic filler from 100 mass parts of resin components in the thermosetting resin composition from the viewpoint of low thermal expansion and moldability. The content is preferably 10 to 300 parts by mass, more preferably 50 to 250 parts by mass, more preferably 100 to 220 parts by mass, and particularly preferably 130 to 200 parts by mass.

(其它成分) 　　熱硬化性樹脂組成物可在不妨礙本發明的效果的範圍內含有下述其它成分：有機填充材料、難燃劑、熱塑性樹脂、紫外線吸收劑、抗氧化劑、光聚合起始劑、螢光增白劑、黏著性提高劑等。(Other components) The thermosetting resin composition may contain the following other components as long as the effects of the present invention are not hindered: organic fillers, flame retardants, thermoplastic resins, ultraviolet absorbers, antioxidants, and photopolymerization initiators , Fluorescent brightener, adhesion improver, etc.

(有機溶劑) 　　從容易製造預浸體的觀點來看，熱硬化性樹脂組成物可製作成含有有機溶劑之清漆的狀態(以下，亦稱為「樹脂清漆」)。 　　作為有機溶劑，可舉例如：甲醇、乙醇、丙醇、丁醇、甲基賽璐蘇、丁基賽璐蘇、丙二醇單甲基醚等醇系溶劑；丙酮、甲基乙基酮、甲基異丁基酮、環己酮等酮系溶劑；乙酸丁酯、丙二醇單甲基醚乙酸酯等酯系溶劑；四氫呋喃等醚系溶劑；甲苯、二甲苯、均三甲苯等芳香族系溶劑；二甲基甲醯胺、二甲基乙醯胺、N-甲基吡咯啶酮等含氮原子溶劑；二甲基亞碸等含硫原子系溶劑等。此等之中，從溶解性及塗佈後的外觀的觀點來看，以酮系溶劑為佳，以甲基乙基酮較佳。 　　有機溶劑可單獨使用1種，且亦可併用2種以上。 　　從處理性的觀點來看，樹脂清漆中的固體成分濃度以10～80質量％為佳，以20～75質量％較佳，以40～75質量％更佳。 　　本說明書中，所謂「固體成分」，是指熱硬化性樹脂組成物中所含的除了水、溶劑等會揮發的物質以外的非揮發成分，是表示在將熱硬化性樹脂組成物乾燥時不會揮發而會殘留的成分，並且，亦包含在25℃附近的室溫為液狀、水飴狀及清漆狀的成分。(Organic Solvent) From the viewpoint of making a prepreg easy, the thermosetting resin composition can be made into a state of a varnish containing an organic solvent (hereinafter, also referred to as "resin varnish"). Examples of the organic solvent include alcohol solvents such as methanol, ethanol, propanol, butanol, methylcellulose, butylcellulose, and propylene glycol monomethyl ether; acetone, methyl ethyl ketone, and methyl alcohol. Ketone solvents such as isobutyl ketone and cyclohexanone; ester solvents such as butyl acetate and propylene glycol monomethyl ether acetate; ether solvents such as tetrahydrofuran; aromatic solvents such as toluene, xylene and mesitylene; Nitrogen atom-containing solvents such as dimethylformamide, dimethylacetamide, and N-methylpyrrolidone; sulfur atom-based solvents such as dimethylsulfine and the like. Among these, from the viewpoint of solubility and appearance after coating, a ketone-based solvent is preferred, and methyl ethyl ketone is preferred. Organic solvents can be used alone or in combination of two or more. From the viewpoint of handleability, the solid content concentration in the resin varnish is preferably 10 to 80% by mass, more preferably 20 to 75% by mass, and even more preferably 40 to 75% by mass. In the present specification, the "solid content" means a non-volatile component other than volatile materials such as water and a solvent contained in the thermosetting resin composition, and means that the thermosetting resin composition is not dried when the thermosetting resin composition is dried. Components that are volatilized and remain, and also include components that are liquid, leeches, and varnishes at room temperature around 25 ° C.

[預浸體的製造方法] 　　其次，說明包含上述步驟1～3之本發明的預浸體的製造方法。[Method for Producing Prepreg] Next, a method for producing a prepreg of the present invention including the above steps 1 to 3 will be described.

＜步驟1＞ 　　步驟1是獲得預浸體前驅物的步驟，並且，前述預浸體前驅物是對熱硬化性樹脂組成物進行B階段化而成，且於前述B階段化中，使熱硬化性樹脂組成物含浸於基材中之後實施加熱處理。<Step 1> Step 1 is a step of obtaining a prepreg precursor, and the prepreg precursor is obtained by subjecting a thermosetting resin composition to a B-stage process, and in the B-stage process, heat curing is performed. After the resin composition is impregnated into the substrate, heat treatment is performed.

作為使熱硬化性樹脂組成物含浸於基材中的方法並無特別限定，可舉例如：熱熔法、溶劑法等。 　　熱熔法為使經藉由加熱來進行低黏度化的熱硬化性樹脂組成物直接含浸於基材中的方法，可舉例如：將熱硬化性樹脂組成物暫時塗佈於剝離性優異的塗佈紙等而形成樹脂薄膜後積層於基材上的方法；使用模具塗佈器等來將熱硬化性樹脂組成物直接塗佈於基材上的方法等。 　　溶劑法是在使熱硬化性樹脂組成物在製作成樹脂清漆的狀態下含浸於基材中的方法，可舉例如：將基材浸漬於樹脂清漆中之後進行乾燥的方法等。The method of impregnating a thermosetting resin composition in a base material is not specifically limited, For example, a hot-melt method, a solvent method, etc. are mentioned. The hot-melt method is a method of directly impregnating a thermosetting resin composition that is reduced in viscosity by heating into a substrate. For example, the thermosetting resin composition is temporarily applied to a coating having excellent peelability. A method in which a resin film is formed by cloth or the like and then laminated on a substrate; a method in which a thermosetting resin composition is directly applied to the substrate using a die coater or the like. The solvent method is a method in which a thermosetting resin composition is impregnated into a substrate in a state of being prepared into a resin varnish, and examples thereof include a method of immersing a substrate in a resin varnish and then drying it.

此處，當應用前述熱熔法時，B階段化可與將前述樹脂薄膜積層於基材上時的加熱同時進行。換言之，能以下述方式對熱硬化性樹脂組成物進行B階段化來獲得預浸體前驅物：將前述樹脂薄膜一面加熱一面積層於基材上，並且在維持此狀態下持續加熱。此時，前述積層時的加熱溫度與進行B階段化時的加熱溫度可相同或不同。 　　此外，當應用前述溶劑法時，B階段化可與將前述樹脂清漆乾燥時的加熱同時進行。換言之，可以下述方式對熱硬化性樹脂組成物進行B階段化來獲得預浸體前驅物：將基材浸漬於樹脂清漆中之後，一面藉由加熱來將有機溶劑乾燥，一面在維持此狀態下持續加熱。此時，前述乾燥時的加熱溫度與進行B階段化時的加熱溫度可相同或不同。 　　本步驟中，加熱處理的條件只要為能夠對熱硬化性樹脂組成物進行B階段化的條件，則無特別限定，只要因應熱硬化性樹脂的種類等來適當決定即可。加熱處理的溫度例如為70～200℃，可為80～150℃，亦可為90～130℃。加熱處理的時間例如為1～30分鐘，可為2～25分鐘，亦可為3～20分鐘。當應用前述熱熔法時，該條件亦能夠稱為積層條件，當應用前述溶劑法時，該條件亦能夠稱為乾燥條件。Here, when the aforementioned hot-melt method is applied, the B-stage conversion can be performed simultaneously with the heating when the aforementioned resin film is laminated on the substrate. In other words, the prepreg precursor can be obtained by performing the B-stage conversion of the thermosetting resin composition in such a manner that the resin film is heated on one side and an area layer on the substrate, and the heating is continued while maintaining this state. In this case, the heating temperature during the lamination may be the same as or different from the heating temperature during the B-stage conversion. In addition, when the aforementioned solvent method is applied, the B-stage conversion can be performed simultaneously with heating when the aforementioned resin varnish is dried. In other words, the precursor of the thermosetting resin composition can be obtained in a B-stage manner by immersing the substrate in a resin varnish and drying the organic solvent by heating while maintaining the state. Under continuous heating. In this case, the heating temperature during the drying and the heating temperature during the B-stage conversion may be the same or different. In this step, the conditions for the heat treatment are not particularly limited as long as they can be B-staged into the thermosetting resin composition, and may be appropriately determined according to the type of the thermosetting resin and the like. The temperature of the heat treatment is, for example, 70 to 200 ° C, 80 to 150 ° C, or 90 to 130 ° C. The heat treatment time is, for example, 1 to 30 minutes, may be 2 to 25 minutes, or may be 3 to 20 minutes. When the aforementioned hot melt method is applied, this condition can also be referred to as a lamination condition, and when the aforementioned solvent method is applied, this condition can also be referred to as a drying condition.

＜步驟2＞ 　　步驟2是將步驟1中獲得的預浸體前驅物冷卻的步驟。換言之，步驟2是針對在步驟1中對預浸體前驅物實施加熱處理而使其進行B階段化而得而獲得的預浸體前驅物，將該預浸體前驅物至少比進行該加熱處理的溫度更低的溫度的步驟。 　　藉由實施本步驟，而會接受熱硬化性樹脂組成物的B階段化及冷卻這樣的在製造預浸體時一般會施加的熱履歷，而所獲得的預浸體前驅物，在其內部存在有習知預浸體會發生的應變等，該應變會成為尺寸變化的主要原因。 　　如上所述，藉由在後述的步驟3之前預先使起因於加熱(步驟1)及冷卻(步驟2)這樣的熱履歷而發生的應變等存在於內部，便能夠有效實現下述：藉由步驟3來消除上述應變等及使尺寸變化量均勻。進一步，由於起因於加熱(步驟1)及冷卻(步驟2)這樣的熱履歷的應變已藉由步驟3來消除，而在步驟3以後即使施加相同的熱履歷亦不會發生應變、或即使發生應變亦非常小，故藉由本發明來獲得的預浸體的尺寸變化量的偏差極小。<Step 2> Step 2 is a step of cooling the prepreg precursor obtained in step 1. In other words, step 2 is directed to the prepreg precursor obtained by subjecting the prepreg precursor to a B-stage heating treatment in step 1, and the prepreg precursor is subjected to the heat treatment at least more than the prepreg precursor. Steps to lower temperatures. By carrying out this step, a thermal history generally applied during the production of a prepreg, such as B-stage conversion and cooling of a thermosetting resin composition, is received, and the obtained prepreg precursor exists in its interior. It is known that the strain which occurs in a prepreg, etc., is a cause of a dimensional change. As described above, by pre-existing the internal strain and the like caused by thermal history such as heating (step 1) and cooling (step 2) before step 3 to be described later, the following can be effectively achieved: 3 to eliminate the above-mentioned strains and the like and make the dimensional change uniform. Further, since the strain caused by thermal history such as heating (step 1) and cooling (step 2) has been eliminated by step 3, after step 3, even if the same thermal history is applied, no strain occurs or even occurs The strain is also very small, so the variation in the dimensional change of the prepreg obtained by the present invention is extremely small.

預浸體前驅物的冷卻可藉由自然放置冷卻來進行，亦可使用送風裝置、冷卻輥等冷卻裝置來進行。本步驟中，冷卻後的預浸體前驅物的表面溫度通常為5～80℃，以8～50℃為佳，以10～30℃較佳，以室溫更佳。 　　再者，本說明書中，所謂室溫，是指未進行加熱、冷卻等溫度控制的環境溫度，一般為15～25℃左右，但由於可能會因天候、季節等而改變，故並不限定於上述範圍內。The cooling of the prepreg precursor can be performed by natural cooling, or a cooling device such as a blower or a cooling roller can be used. In this step, the surface temperature of the cooled prepreg precursor is usually 5 to 80 ° C, preferably 8 to 50 ° C, more preferably 10 to 30 ° C, and more preferably room temperature. In addition, in this specification, the room temperature refers to an ambient temperature without temperature control such as heating and cooling, and is generally about 15 to 25 ° C. However, since it may change due to weather, season, etc., it is not limited to Within the above range.

＜步驟3＞ 　　步驟3是獲得預浸體的步驟，並且，前述預浸體是對在步驟2中冷卻後的預浸體前驅物實施表面加熱處理來獲得，且前述表面加熱處理是使預浸體前驅物的表面溫度上升的處理。<Step 3> Step 3 is a step of obtaining a prepreg, and the prepreg is obtained by subjecting the prepreg precursor cooled in step 2 to a surface heating treatment, and the surface heating treatment is a prepreg A treatment for increasing the surface temperature of a body precursor.

本發明的預浸體藉由實施步驟3，特別是尺寸變化量的偏差會較小。其理由雖尚不明確，但被認為：藉由本步驟，而能夠消除在步驟1、步驟2等之中所產生的預浸體前驅物中的基材的應變，而能夠減少源自該應變的硬化時的尺寸變化，因此，能夠使尺寸變化量均勻。 　　步驟3中，表面加熱處理的加熱方法無特別限制，可舉例如：使用平板加熱器的加熱方法、藉由熱風的加熱方法、藉由高頻的加熱方法、藉由磁力線的加熱方法、藉由雷射的加熱方法、將此等組合而成的加熱方法等。 　　表面加熱處理的加熱條件是預浸體前驅物的表面溫度會較實施表面加熱處理之前的表面溫度更加上升的條件，且只要在不會對所獲得的預浸體的各種特性(例如流動性)造成顯著影響的範圍內，則無特別限定，只要因應熱硬化性樹脂的種類等來適當決定即可。 　　從一面使預浸體的成形性保持良好一面減少尺寸變化量的偏差的觀點來看，由表面加熱處理所造成的預浸體前驅物的表面溫度的上升值(亦即，表面加熱處理前的表面溫度與在表面加熱處理中所到達的最高表面溫度之間的差值的絕對值)以5～110℃為佳，以20～90℃較佳，以40～70℃更佳。 　　從一面使預浸體的成形性保持良好一面減少尺寸變化量的偏差的觀點來看，作為表面加熱處理的加熱溫度，例如為在成為20～130℃的範圍內，較佳是在成為40～110℃的範圍內，更佳是在成為60～90℃的範圍內。 　　此外，從使預浸體的生產性保持良好的觀點、及將預浸體保持在B階段狀態而一面使成形性保持良好一面減少尺寸變化量的偏差的觀點來看，表面加熱處理較佳是在比在步驟1中進行B階段化時的加熱更高溫且更短時間內進行。從該觀點來看，表面加熱處理較佳是在200～700℃的環境中進行，更佳是在250～600℃的環境中進行，進一步更佳是在350～550℃的環境中進行。具體例可舉例如：當實施使用平板加熱器的加熱方法時，平板加熱器的加熱設定溫度以200～700℃為佳，以250～600℃較佳，以350～550℃更佳。 　　從使預浸體的生產性保持良好的觀點、及將預浸體保持在B階段狀態而一面使成形性保持良好一面減少尺寸變化量的偏差的觀點來看，表面加熱處理的加熱時間以1.0～10.0秒為佳，以1.5～6.0秒較佳，以2.0～4.0秒更佳。By performing step 3 of the prepreg of the present invention, in particular, the variation in the amount of dimensional change will be small. Although the reason for this is not clear, it is thought that this step can eliminate the strain of the substrate in the prepreg precursor generated in step 1, step 2 and the like, and can reduce the strain derived from the strain. Since the dimensional change during curing, the amount of dimensional change can be made uniform. In step 3, the heating method for the surface heating treatment is not particularly limited, and examples thereof include a heating method using a flat plate heater, a heating method using hot air, a heating method using high frequency, a heating method using magnetic field lines, and A laser heating method, a heating method combining these, and the like. The heating conditions for the surface heating treatment are conditions in which the surface temperature of the precursor of the prepreg will rise more than the surface temperature before the surface heating treatment is performed, and as long as it does not affect various characteristics (such as flowability) of the obtained prepreg The range that has a significant influence is not particularly limited, and may be appropriately determined depending on the type of the thermosetting resin and the like. From the viewpoint of reducing the variation in the amount of dimensional change while maintaining the formability of the prepreg, the value of the rise in the surface temperature of the prepreg precursor caused by the surface heating treatment (that is, the value before the surface heating treatment) The absolute value of the difference between the surface temperature and the highest surface temperature reached during the surface heating treatment is preferably 5 to 110 ° C, more preferably 20 to 90 ° C, and even more preferably 40 to 70 ° C. From the viewpoint of reducing the variation in the amount of dimensional change while maintaining the moldability of the prepreg, the heating temperature for the surface heating treatment is, for example, in the range of 20 to 130 ° C, and preferably 40 to In the range of 110 ° C, it is more preferably in the range of 60 to 90 ° C. In addition, from the viewpoint of maintaining good productivity of the prepreg and the viewpoint of keeping the prepreg in a B-stage state while maintaining good formability while reducing variations in the amount of dimensional change, the surface heat treatment is preferably The heating is performed at a higher temperature and in a shorter period of time than when heating in the B stage in step 1. From this viewpoint, the surface heating treatment is preferably performed in an environment of 200 to 700 ° C, more preferably in an environment of 250 to 600 ° C, and even more preferably in an environment of 350 to 550 ° C. Specific examples include: when a heating method using a flat plate heater is implemented, the heating set temperature of the flat plate heater is preferably 200 to 700 ° C, more preferably 250 to 600 ° C, and more preferably 350 to 550 ° C. From the viewpoint of maintaining the productivity of the prepreg and maintaining the prepreg in the B-stage state while maintaining the formability while reducing the variation in the amount of dimensional change, the heating time of the surface heating treatment is 1.0. It is preferably -10.0 seconds, more preferably 1.5-6.0 seconds, and even more preferably 2.0-4.0 seconds.

從預浸體的處理性及沾黏性的觀點來看，步驟3中獲得的預浸體較佳是提供至將此預浸體冷卻的冷卻步驟中。預浸體的冷卻可藉由自然放置冷卻來進行，亦可使用送風裝置、冷卻輥等冷卻裝置來進行。冷卻後的預浸體的溫度通常為5～80℃，以8～50℃為佳，以10～30℃較佳，以室溫更佳。From the viewpoint of handleability and stickiness of the prepreg, the prepreg obtained in step 3 is preferably provided to a cooling step of cooling the prepreg. The cooling of the prepreg may be performed by natural cooling, or a cooling device such as a blower or a cooling roll may be used. The temperature of the prepreg after cooling is usually 5 to 80 ° C, preferably 8 to 50 ° C, more preferably 10 to 30 ° C, and even more preferably room temperature.

再者，步驟3可在後述的本發明的覆金屬積層板的製造步驟中實施。具體而言，可在於步驟2中獲得的預浸體前驅物的雙面上配置有金屬箔的狀態下實施步驟3，然後將預浸體及金屬箔積層並進行成形。積層並進行成形的條件等，是如同後述本發明的積層板的項目中所記載。In addition, step 3 can be implemented in the manufacturing process of the metal-clad laminated board of this invention mentioned later. Specifically, step 3 may be performed in a state where metal foils are arranged on both sides of the prepreg precursor obtained in step 2, and then the prepreg and metal foil are laminated and formed. The conditions and the like for laminating and molding are as described in the item of the laminated plate of the present invention described later.

本發明的預浸體中，熱硬化性樹脂組成物的以固體成分來換算的含量以20～90質量％為佳，以30～80質量％較佳，以40～75質量％更佳。 　　本發明的預浸體的厚度例如為0.01～0.5 mm，從成形性及能夠高密度佈線的觀點來看，以0.02～0.2 mm為佳，以0.03～0.1 mm較佳。In the prepreg of the present invention, the content of the thermosetting resin composition in terms of solid content is preferably 20 to 90% by mass, more preferably 30 to 80% by mass, and even more preferably 40 to 75% by mass.的 The thickness of the prepreg of the present invention is, for example, 0.01 to 0.5 mm. From the viewpoint of moldability and high-density wiring, it is preferably 0.02 to 0.2 mm, and more preferably 0.03 to 0.1 mm.

以上述方式獲得的本發明的預浸體的依照下述方法來求出的標準偏差σ以0.012％以下為佳，以0.011％以下較佳，以0.010％以下更佳，以0.009％以下進一步更佳，特佳是0.008％以下。標準偏差σ的下限值無特別限制，通常為0.003％以上，可為0.005％以上，且亦可為0.006％以上，且亦可為0.007％以上。 　標準偏差σ的算出方法： 　　將厚度18 μm的銅箔重疊在1片預浸體的雙面上，並以190℃、2.45 MPa的條件進行90分鐘的加熱加壓成形，來製作厚度0.1 mm的雙面覆銅積層板；對於以上述方式獲得的雙面覆銅積層板，在該雙面覆銅積層板的面內的在第1圖中所記載的1～8處實施直徑1.0 mm的開孔。對在第1圖中所記載的縱線方向也就是1-7、2-6、3-5的方向及橫線方向也就是1-3、8-4、7-5的方向的各3點，使用影像測定機來對各3點之間的距離進行測定後，將各測定距離設為初期值；然後，將外層銅箔去除，並利用乾燥機以185℃加熱60分鐘；冷卻後，以與初期值的測定方法相同之方式，來對縱線方向也就是1-7、2-6、3-5的方向及橫線方向也就是1-3、8-4、7-5的方向的各3點之間的距離進行測定；根據相對於各測定距離的初期值的變化率[(加熱處理後的測定值－初期值)×100/初期值]來求出該等變化率的平均值，並算出相對於該平均值的標準偏差σ。 　　前述影像測定機並無特別限定，能夠使用例如「QV-A808P1L-D」(Mitutoyo公司製)。The standard deviation σ of the prepreg of the present invention obtained in the above manner obtained in accordance with the following method is preferably 0.012% or less, more preferably 0.011% or less, more preferably 0.010% or less, and even more preferably 0.009% or less. Good, particularly good is 0.008% or less. The lower limit value of the standard deviation σ is not particularly limited, but is usually 0.003% or more, may be 0.005% or more, and may be 0.006% or more, and may be 0.007% or more. Method for calculating standard deviation σ: Overlay copper foil with a thickness of 18 μm on both sides of one prepreg, and heat-press for 90 minutes at 190 ° C and 2.45 MPa to produce a 0.1 mm thickness. Double-sided copper-clad laminated board; for the double-sided copper-clad laminated board obtained in the above manner, openings of 1.0 mm in diameter were performed at 1 to 8 locations shown in the first figure in the plane of the double-sided copper-clad laminated board. hole. For each of the three points in the direction of the vertical line described in Figure 1, that is, the direction of 1-7, 2-6, 3-5, and the direction of the horizontal line, that is, 1-3, 8-4, and 7-5 After measuring the distance between each three points using an image measuring machine, set each measuring distance to an initial value; then, remove the outer layer of copper foil and heat it at 185 ° C for 60 minutes with a dryer; after cooling, use In the same way as the initial value measurement method, the vertical direction is the direction of 1-7, 2-6, 3-5, and the horizontal direction is the direction of 1-3, 8-4, 7-5. The distance between each three points is measured; the average value of these rates of change is obtained from the rate of change [(measured value after heat treatment-initial value) × 100 / initial value] relative to the initial value of each measured distance And calculate the standard deviation σ from the average. The image measuring machine is not particularly limited, and for example, "QV-A808P1L-D" (manufactured by Mitutoyo) can be used.

[積層板] 　　本發明的積層板是將本發明的預浸體與金屬箔積層並進行成形而成。 　　本發明的積層板能夠藉由例如下述方式來製造：以使用1片本發明的預浸體或因應需要來將本發明的預浸體重疊2～20片並於其單面或雙面上配置有金屬箔的構成來積層並進行成形。再者，有時將配置有金屬箔之積層板稱為覆金屬積層板。[Laminated Sheet] 的 The laminated sheet of the present invention is formed by laminating and forming a prepreg of the present invention and a metal foil. The laminated board of the present invention can be manufactured, for example, by using one sheet of the prepreg of the present invention or, if necessary, overlapping the prepreg of the present invention by 2 to 20 sheets and placing it on one or both sides. A metal foil structure is arranged to be laminated and formed. In addition, a laminated board in which a metal foil is arranged may be referred to as a metal-clad laminated board.

金屬箔的金屬只要為電絕緣材料用途中所使用的金屬，則無特別限制。 　　從導電性的觀點來看，作為金屬箔的金屬，較佳是銅、金、銀、鎳、鉑、鉬、釕、鋁、鎢、鐵、鈦、鉻、包含此等金屬元素之中的至少1種的合金，以銅、鋁較佳，以銅更佳。換言之，本發明的積層板以覆銅積層板為佳。 　　金屬箔的厚度只要依印刷線路板的用途等來適當選擇即可，以0.5～150 μm為佳，以1～100 μm較佳，以5～50 μm更佳，以5～30 μm特佳。 　　此外，可藉由對金屬箔進行鍍覆來形成鍍覆層。鍍覆層的金屬只要為能夠用於進行鍍覆的金屬，則無特別限制，較佳是銅、金、銀、鎳、鉑、鉬、釕、鋁、鎢、鐵、鈦、鉻、包含此等金屬元素之中的至少1種的合金。 　　作為鍍覆方法並無特別限制，能夠利用：電解鍍覆法、無電解鍍覆法。The metal of the metal foil is not particularly limited as long as it is a metal used for an electrical insulating material application. From the viewpoint of conductivity, the metal of the metal foil is preferably copper, gold, silver, nickel, platinum, molybdenum, ruthenium, aluminum, tungsten, iron, titanium, chromium, and contains at least one of these metal elements. One type of alloy is preferably copper and aluminum, and more preferably copper. In other words, the laminated board of the present invention is preferably a copper-clad laminated board. The thickness of the metal foil may be appropriately selected according to the use of the printed wiring board, etc., preferably 0.5 to 150 μm, more preferably 1 to 100 μm, more preferably 5 to 50 μm, and particularly preferably 5 to 30 μm. In addition, a plated layer can be formed by plating a metal foil. The metal of the plating layer is not particularly limited as long as it can be used for plating. Copper, gold, silver, nickel, platinum, molybdenum, ruthenium, aluminum, tungsten, iron, titanium, chromium, and the like are included. An alloy of at least one of the equal metal elements. There is no particular limitation on as a plating method, and an electrolytic plating method or an electroless plating method can be used.

作為積層板的成形條件，能夠應用電絕緣材料用積層板及多層板的習知成形手法，能夠例如：使用多段加壓、多段真空加壓、連續成形、高壓釜成形機等，在溫度100～250℃、壓力0.2～10 MPa、加熱時間0.1～5小時的條件下成形。 　　此外，亦能夠將本發明的預浸體與內層用印刷線路板組合且積層並進行成形來製造多層板。As the forming conditions of the laminated board, a conventional forming method for laminated boards for electric insulating materials and multilayer boards can be applied. For example, multi-stage pressure, multi-stage vacuum pressure, continuous forming, autoclave forming machine, etc. can be used at a temperature of 100 to It is molded under the conditions of 250 ° C, a pressure of 0.2 to 10 MPa, and a heating time of 0.1 to 5 hours. In addition, the prepreg of the present invention and a printed wiring board for an inner layer can be combined and laminated to form a multilayer board.

[印刷線路板] 　　本發明的印刷線路板是包含本發明的預浸體或本發明的積層板而成。 　　本發明的印刷線路板能夠藉由例如下述方式來製造：對本發明的積層板的金屬箔實施電路加工。電路加工能夠藉由例如下述方式來進行：於金屬箔表面形成阻劑圖案後，藉由蝕刻來將多餘部分的金屬箔去除，並將阻劑圖案剝離後，藉由鑽頭或雷射來形成需要的貫穿孔，並再次形成阻劑圖案後，對貫穿孔實施用以導通的鍍覆，最後將阻劑圖案剝離。 　　能夠以下述方式製作成多層印刷線路板：在與前述相同的條件下進一步將上述覆金屬積層板積層於以上述方式獲得的印刷線路板的表面，並進一步與上述同樣地進行而進行電路加工。此時，不一定必須形成貫穿孔，亦可形成通孔，且亦可形成該等雙方。這樣的多層化只要進行需要的片數即可。[Printed wiring board] The printed wiring board of the present invention includes a prepreg of the present invention or a laminated board of the present invention.印刷 The printed wiring board of the present invention can be manufactured, for example, by subjecting the metal foil of the laminated board of the present invention to circuit processing. The circuit processing can be performed, for example, by forming a resist pattern on the surface of the metal foil, removing excess metal foil by etching, peeling the resist pattern, and then forming the resist pattern by a drill or a laser. After the required through-holes are formed and the resist pattern is formed again, the through-holes are plated for conduction, and finally the resist pattern is peeled off.多层 A multilayer printed wiring board can be produced by further laminating the metal clad laminate on the surface of the printed wiring board obtained in the above manner under the same conditions as described above, and further performing circuit processing in the same manner as described above. In this case, it is not necessary to form a through hole, a through hole may be formed, and both of them may be formed. Such multi-layering may be performed by a required number of sheets.

[半導體封裝體] 　　本發明的半導體封裝體是使用本發明的印刷線路板而成。 　　本發明的半導體封裝體能夠以下述方式製造：將半導體晶片、記憶體等安裝在本發明的印刷線路板的既定位置上。 [實施例][Semiconductor Package] (1) The semiconductor package of the present invention is obtained by using the printed wiring board of the present invention.半导体 The semiconductor package of the present invention can be manufactured by mounting a semiconductor wafer, a memory, and the like on a predetermined position of the printed wiring board of the present invention. [Example]

其次，藉由下述實施例來更詳細地說明本發明，但此等實施例在任何意義上皆並非用以限制本發明。各例中所獲得的預浸體等是依照下述評估方法來評估性能。再者，本實施例中的室溫為25℃。Next, the present invention is described in more detail by the following examples, but these examples are not intended to limit the present invention in any sense. The prepregs and the like obtained in each example were evaluated for performance in accordance with the following evaluation methods. The room temperature in this example is 25 ° C.

[評估方法] ＜1.成形性＞ 　　對將各例中所製得的四層覆銅積層板浸漬於蝕刻液中來將外層銅去除而獲得的評估基板，以肉眼來確認340 mm×500 mm的面內有無孔洞及擦傷。將無法確認有孔洞及擦傷設為「無異常」，將能夠確認有孔洞及擦傷設為「有異常」，來作為成形性的指標。[Evaluation method] <1. Formability> The evaluation substrate obtained by immersing the four-layer copper-clad laminated board prepared in each example in an etching solution to remove the outer layer of copper was confirmed with the naked eye 340 mm × 500 mm There are no holes or abrasions in the face. The holes and abrasions that cannot be confirmed are set to "no abnormality", and the holes that can be confirmed and abrasions are set to "with abnormality" as indicators of formability.

＜2.尺寸變化量的偏差＞ 　　對各例中所製得的雙面覆銅積層板的面內，像第1圖所示這樣進行直徑1.0 mm的開孔，而獲得第1圖的概略圖中表示的評估基板。 　　然後，使用「QV-A808P1L-D」(Mitutoyo股份有限公司製)來對第1圖中的「縱線方向」的各3點之間孔間距離(1-7間、2-6間、3-5間)及「橫線方向」的各3點之間孔間距離(1-3間、8-4間、7-5間)進行測定後，將各測定距離設為初期值。然後，將評估基板浸漬於蝕刻液中來將外層銅去除後，使用乾燥機來在185℃加熱60分鐘。冷卻後，藉由與初期值相同的方法來測定各孔間距離後，設為加熱處理後的測定值。 　　對各孔間距離，求出加熱處理後的測定值相對於初期值的變化率[(初期值－加熱處理後的測定值)×100/初期值]，並算出相對於該等的平均值的標準偏差σ後，將該標準偏差σ設為尺寸變化量的偏差。<2. Variation in dimensional change> In the plane of the double-sided copper-clad laminates prepared in each example, a hole with a diameter of 1.0 mm was opened as shown in Fig. 1 to obtain a schematic diagram of Fig. 1 The evaluation substrate shown in. Then, using "QV-A808P1L-D" (manufactured by Mitutoyo Co., Ltd.), the distance between the three holes (1-7, 2-6, 3 -5) and the distance between the holes (1-3, 8-4, and 7-5) between the three points in the "horizontal direction", and then set each measurement distance as the initial value. Then, the evaluation substrate was immersed in an etching solution to remove the outer layer of copper, and then heated at 185 ° C. for 60 minutes using a dryer. After cooling, the distance between each hole was measured by the same method as the initial value, and it was set as the measured value after heat processing. For each of the distances between the holes, the rate of change of the measured value after the heat treatment relative to the initial value [(initial value-measured value after the heat treatment) × 100 / initial value] was calculated, and the average value of these values was calculated. After the standard deviation σ, the standard deviation σ is taken as the deviation of the dimensional change.

[實施例1] (預浸體前驅物的製作：步驟1～2) 　　藉由將下述混合並以溶劑(甲基乙基酮)來稀釋，而調製清漆狀的熱硬化性樹脂組成物(固體成分濃度：70質量％)。 　作為(A)熱硬化性樹脂的聯苯芳烷基酚醛清漆型環氧樹脂(環氧當量：280～300 g/eq)19質量份； 　作為(B)硬化劑的甲酚酚醛清漆樹脂(羥基當量：119 g/eq)16質量份； 　作為(C)硬化促進劑的2-乙基-4-甲基咪唑(四國化成工業股份有限公司製)0.02質量份； 　作為(D)無機填充材料的球狀氧化矽(平均粒徑：2 μm)65質量份。 　　使此熱硬化性樹脂組成物含浸於基材亦即玻璃布(日東紡績股份有限公司製，商品名：1037布，厚度：0.025 mm)後，在乾燥爐內在100～200℃加熱5～15分鐘直到熱硬化性樹脂組成物B階段化為止。然後，藉由自然放置冷卻來冷卻至室溫，而獲得預浸體前驅物。[Example 1] (Preparation of prepreg precursor: steps 1 to 2) A varnish-like thermosetting resin composition was prepared by mixing the following and diluting with a solvent (methyl ethyl ketone) ( Solid content concentration: 70% by mass). 19 parts by mass of a biphenylaralkyl novolac type epoxy resin (epoxy equivalent: 280 to 300 g / eq) as (A) a thermosetting resin; 的 cresol novolac resin (hydroxyl group) as a (B) curing agent Equivalent: 119 g / eq) 16 parts by mass; 0.02 0.02 parts by mass of 2-ethyl-4-methylimidazole (manufactured by Shikoku Chemical Industry Co., Ltd.) as (C) hardening accelerator; as (D) inorganic filler 65 parts by mass of spherical silica (average particle diameter: 2 μm). This thermosetting resin composition was impregnated with glass cloth (made by Nitto Textile Co., Ltd., trade name: 1037 cloth, thickness: 0.025 mm), and then heated in a drying furnace at 100 to 200 ° C. for 5 to 15 minutes. Until the thermosetting resin composition becomes B-stage. Then, it was cooled to room temperature by leaving it to cool naturally to obtain a prepreg precursor.

(預浸體的製作：步驟3) 　　對上述中獲得的預浸體前驅物，使用平板加熱器，以加熱設定溫度500℃、使預浸體前驅物的表面溫度成為70℃、加熱時間3秒的條件下，實施表面加熱處理後，冷卻至室溫，而獲得預浸體。 　　再者，所獲得的預浸體中，熱硬化性樹脂組成物的以固體成分來換算的含量為70質量％。(Preparation of prepreg: Step 3) The prepreg precursor obtained in the above was heated using a flat plate heater at a set temperature of 500 ° C, the surface temperature of the prepreg precursor was 70 ° C, and the heating time was 3 seconds. After the surface is subjected to a heat treatment under the conditions described above, it is cooled to room temperature to obtain a prepreg. Furthermore, the content of the thermosetting resin composition in terms of solid content in the obtained prepreg was 70% by mass.

(覆銅積層板的製作) 　　使用1片上述中所獲得的預浸體，將18 μm銅箔「YGP-18」(日本電解股份有限公司製)重疊在其雙面上，並以溫度190℃、壓力25 kgf/cm2 (2.45 MPa)加熱加壓成形90分鐘，而製作預浸體1片份的雙面覆銅積層板。 　　對所獲得的雙面覆銅積層板的兩個銅箔面實施內層密合處理(使用「BF處理液」(日立化成股份有限公司製))後，各重疊1片預浸體，且將18 μm銅箔「YGP-18」(日本電解股份有限公司製)重疊在其雙面上，並以溫度190℃、壓力25 kgf/cm2 (2.45 MPa)加熱加壓成形90分鐘，而製作四層覆銅積層板。 　　另一方面，將18 μm銅箔「3EC-VLP-18」(三井金屬股份有限公司製)重疊在1片預浸體的雙面上，並以溫度190℃、壓力25 kgf/cm2 (2.45 MPa)加熱加壓成形90分鐘，而製作預浸體1片份的雙面覆銅積層板。(Production of copper-clad laminated board) Using one piece of the prepreg obtained above, 18 μm copper foil "YGP-18" (manufactured by Japan Electrolytic Corporation) was superposed on both sides, and the temperature was 190 ° C. A pressure of 25 kgf / cm 2 (2.45 MPa) was heated and press-molded for 90 minutes to prepare a double-sided copper-clad laminated board of 1 part of prepreg. Two copper foil surfaces of the obtained double-sided copper-clad laminated board were subjected to inner layer adhesion treatment (using a "BF treatment liquid" (manufactured by Hitachi Chemical Co., Ltd.)), and then one prepreg was superimposed on each other, and 18 μm copper foil "YGP-18" (manufactured by Japan Electrolytic Co., Ltd.) was superposed on both sides, and heated and press-molded at a temperature of 190 ° C and a pressure of 25 kgf / cm 2 (2.45 MPa) for 90 minutes. Laminated copper laminates. On the other hand, 18 μm copper foil "3EC-VLP-18" (manufactured by Mitsui Metals Co., Ltd.) was superposed on both sides of a single prepreg, and the temperature was 190 ° C and the pressure was 25 kgf / cm 2 (2.45 MPa) was heated and press-molded for 90 minutes to prepare a double-sided copper-clad laminated board of one piece of prepreg.

[實施例2] (預浸體前驅物的製作：步驟1～2) 　(A)成分：使用下述製造例1中所製得的馬來醯亞胺化合物(A)的溶液。 [製造例1] 　　在具備溫度計、攪拌裝置及裝有回流冷卻管的水分定量器之容積1 L反應容器中，加入4,4’-二胺基二苯基甲烷19.2 g、雙(4-馬來醯亞胺基苯基)甲烷174.0 g、對胺基苯酚6.6 g及二甲基乙醯胺330.0 g，並在100℃使其進行反應2小時，而獲得具有酸性取代基及N-取代馬來醯亞胺基之馬來醯亞胺化合物(A)(Mw＝1,370)之二甲基乙醯胺溶液，並作為(A)成分使用。 　　再者，上述重量平均分子量(Mw)是藉由凝膠滲透層析法(GPC)，根據使用標準聚苯乙烯的校準曲線換算。校準曲線是使用標準聚苯乙烯：TSK standard POLYSTYRENE(型號：A-2500、A-5000、F-1、F-2、F-4、F-10、F-20、F-40)[東曹股份有限公司製]以三次方程式來進行近似。GPC的條件是如下所示。 　裝置：(泵：L-6200型[日立High-Technologies股份有限公司製])、 　　　(偵測器：L-3300型RI[日立High-Technologies股份有限公司製])、 　　　(管柱烘箱：L-655A-52[日立High-Technologies股份有限公司製]) 　管柱：TSKgel SuperHZ2000＋TSKgel SuperHZ2300(皆為東曹股份有限公司製) 　管柱大小：6.0 mm×40 mm(保護管柱)，7.8×300 mm(管柱) 　溶析液：四氫呋喃 　樣品濃度：20 mg/5 mL 　注入量：10 μL 　流量：0.5 mL/分鐘 　測定溫度：40℃[Example 2] (Preparation of prepreg precursor: Steps 1 to 2) Component (A): A solution of the maleimidine imine compound (A) prepared in the following Production Example 1 was used. [Manufacturing Example 1] (1) A reaction vessel having a volume of 1 L equipped with a thermometer, a stirring device, and a water content meter equipped with a reflux cooling pipe was charged with 19.2 g of 4,4'-diaminodiphenylmethane and bis (4-Ma 174.0 g of lyliminophenyl) methane, 6.6 g of p-aminophenol and 330.0 g of dimethylacetamide, and reacted at 100 ° C for 2 hours to obtain an acidic substituent and an N-substituted horse A dimethylacetamide solution of the maleimide compound (A) (Mw = 1,370) of lylimidine, and used as (A) component. Furthermore, the weight average molecular weight (Mw) is converted by a gel permeation chromatography (GPC) according to a calibration curve using standard polystyrene. The calibration curve is using standard polystyrene: TSK standard POLYSTYRENE (model: A-2500, A-5000, F-1, F-2, F-4, F-10, F-20, F-40) [东 曹Co., Ltd.] is approximated by a cubic equation. The conditions of GPC are as follows. Device: (pump: L-6200 [Hitachi High-Technologies Co., Ltd.]), (detector: L-3300 RI [Hitachi High-Technologies Co., Ltd.]), (column oven: L- 655A-52 [manufactured by Hitachi High-Technologies Co., Ltd.]) column: TSKgel SuperHZ2000 + TSKgel SuperHZ2300 (both manufactured by Tosoh Corporation) 大小 column size: 6.0 mm × 40 mm (protective column), 7.8 × 300 mm ( (Column) Eluent: Tetrahydrofuran Sample concentration: 20 mg / 5 mL Injection volume: 10 μL Flow rate: 0.5 mL / min Measurement temperature: 40 ° C

以成為下述的方式調配(其中，當為溶液時是表示以固體成分來換算的量)，並進一步以使溶液的固體成分濃度成為65～75質量％的方式額外加入甲基乙基酮，而調製樹脂清漆。 　作為(A)熱硬化性樹脂的上述中所獲得的馬來醯亞胺化合物(A)45質量份、及甲酚酚醛清漆型環氧樹脂30質量份； 　作為(B)成分的雙氰胺(日本CARBIDE工業股份有限公司製)2質量份； 　作為(D)成分的經藉由胺基矽烷系耦合劑來進行處理後的熔融氧化矽(平均粒徑：1.9 μm，比表面積5.8 m2 /g)50質量份； 　作為熱塑性樹脂的苯乙烯與馬來酸酐的共聚樹脂(苯乙烯/馬來酸酐＝4，Mw＝11,000)25質量份； 　作為難燃劑的芳香族磷酸酯以磷原子來換算的量為2.0質量份。 　　使所獲得的各樹脂清漆含浸於IPC規格＃3313的玻璃布(0.1 mm)中，並使用設定在溫度160℃的平板加熱器來乾燥4分鐘(步驟1)後，在室溫放置冷卻(步驟2)，而獲得預浸體前驅物。Blend it as follows (where it is a solution, it means the amount converted by solid content), and further add methyl ethyl ketone so that the solid content concentration of the solution becomes 65 to 75% by mass, And modulation resin varnish. (A) 45 parts by mass of the maleimide compound (A) obtained as described above and 30 parts by mass of a cresol novolak-type epoxy resin; dicyandiamide (B) as a component ( 2 parts by mass of Japan Carbide Industrial Co., Ltd .; Fused silica (average particle diameter: 1.9 μm, specific surface area: 5.8 m 2 / g) after being treated with an aminosilane-based coupling agent as component (D) ) 50 parts by mass; 25 parts by mass of a copolymer resin of styrene and maleic anhydride (styrene / maleic anhydride = 4, Mw = 11,000) as a thermoplastic resin; an aromatic phosphate ester as a flame retardant converted by a phosphorus atom The amount is 2.0 parts by mass. Each obtained resin varnish was impregnated in glass cloth (0.1 mm) of IPC specification # 3313, and dried using a flat plate heater set at a temperature of 160 ° C for 4 minutes (step 1), and then left to cool at room temperature (step 2) to obtain a prepreg precursor.

(預浸體的製作：步驟3) 　　對上述中所獲得的預浸體前驅物，使用平板加熱器，以加熱設定溫度500℃、使預浸體前驅物的表面溫度成為70℃、加熱時間3秒的條件下，實施表面加熱處理後，冷卻至室溫，而獲得預浸體。 　　再者，所獲得的預浸體中，熱硬化性樹脂組成物的以固體成分來換算的含量為70質量％。(Preparation of prepreg: Step 3) The prepreg precursor obtained in the above was heated using a flat plate heater at a set temperature of 500 ° C, the surface temperature of the prepreg precursor was 70 ° C, and the heating time was 3 After performing the surface heating treatment under the conditions of seconds, it was cooled to room temperature to obtain a prepreg. Furthermore, the content of the thermosetting resin composition in terms of solid content in the obtained prepreg was 70% by mass.

(覆銅積層板的製作) 　　使用1片上述中所獲得的預浸體，並與實施例1同樣地進行，而製作四層覆銅積層板及雙面覆銅積層板。(Production of copper-clad laminated board) Using one piece of the prepreg obtained above, the same procedure as in Example 1 was performed to produce a four-layer copper-clad laminated board and a double-sided copper-clad laminated board.

[比較例1] 　　除了在實施例1中不實施步驟3的點以外，其餘與實施例1同樣地進行，而製作四層覆銅積層板及雙面覆銅積層板。[Comparative Example 1] Except for the point that Step 3 was not carried out in Example 1, the same procedure as in Example 1 was performed to produce a four-layer copper-clad laminate and a double-sided copper-clad laminate.

[比較例2] 　　除了在實施例2中不實施步驟3的點以外，其餘與實施例1同樣地進行，而製作四層覆銅積層板及雙面覆銅積層板。[Comparative Example 2] Except for the point that Step 3 was not performed in Example 2, the same procedure as in Example 1 was performed to produce a four-layer copper-clad laminate and a double-sided copper-clad laminate.

上述各例中所獲得的四層覆銅積層板及雙面覆銅積層板的評估結果是如表1所示。The evaluation results of the four-layer copper-clad laminates and the double-sided copper-clad laminates obtained in the above examples are shown in Table 1.

[表1] [Table 1]

實施例1及2的預浸體，在成形性方面，樹脂的填埋性良好，而在由此預浸體所獲得的積層板中，無法確認有擦傷、孔洞等異常。此外，與未進行表面加熱處理的比較例1及2的預浸體相比，實施例1及2的預浸體，顯示出尺寸變化量的偏差(標準偏差(σ))有減少的傾向。 [產業上的可利用性]The prepregs of Examples 1 and 2 had good landfillability of the resin in terms of moldability. However, in the multilayer board obtained from the prepreg, abnormalities such as scratches and holes were not confirmed. In addition, the prepregs of Examples 1 and 2 showed a tendency to reduce the variation (standard deviation (σ)) in the amount of dimensional change compared to the prepregs of Comparative Examples 1 and 2 that were not subjected to the surface heating treatment. [Industrial availability]

本發明的預浸體由於成形性優異且尺寸變化量較小，故有用於作為經高積體化的半導體封裝體、電子機器用印刷線路板等。The prepreg of the present invention is excellent in formability and has a small amount of dimensional change, and is therefore useful as a semiconductor package, a printed wiring board for an electronic device, and the like, which are highly integrated.

第1圖是在實施例中測定尺寸變化量的偏差時所使用的評估基板的概略圖。FIG. 1 is a schematic diagram of an evaluation substrate used when measuring the variation in the amount of dimensional change in the examples.

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Claims (10)

一種預浸體，其經過下述步驟1～3來獲得： 　　步驟1：獲得預浸體前驅物的步驟，並且，前述預浸體前驅物是對熱硬化性樹脂組成物進行B階段化而成，且於前述B階段化中，使熱硬化性樹脂組成物含浸於基材中之後實施加熱處理； 　　步驟2：將步驟1中獲得的預浸體前驅物冷卻的步驟； 　　步驟3：獲得預浸體的步驟，並且，前述預浸體是對在步驟2中冷卻後的預浸體前驅物實施表面加熱處理來獲得，且前述表面加熱處理是使預浸體前驅物的表面溫度上升的處理。A prepreg is obtained through the following steps 1-3: Step 1: A step of obtaining a prepreg precursor, and the prepreg precursor is obtained by subjecting a thermosetting resin composition to a B-stage process. In step B, the thermosetting resin composition is impregnated in the substrate and then subjected to a heat treatment; Step 2: a step of cooling the prepreg precursor obtained in Step 1; Step 3: Obtaining a prepreg The prepreg is obtained by subjecting the prepreg precursor cooled in step 2 to a surface heating treatment, and the surface heating treatment is a treatment for increasing the surface temperature of the prepreg precursor. 如請求項1所述之預浸體，其中，步驟3中的表面加熱處理是使前述預浸體前驅物的表面溫度上升5～110℃的處理。The prepreg according to claim 1, wherein the surface heating treatment in step 3 is a treatment for increasing the surface temperature of the prepreg precursor by 5 to 110 ° C. 如請求項1或2所述之預浸體，其中，步驟3中的表面加熱處理是將前述預浸體前驅物的表面溫度加熱至20～130℃的處理。The prepreg according to claim 1 or 2, wherein the surface heating treatment in step 3 is a treatment in which the surface temperature of the prepreg precursor is heated to 20 to 130 ° C. 如請求項1至3中任一項所述之預浸體，其中，步驟3中的表面加熱處理是在200～700℃的環境中將前述預浸體前驅物加熱的處理。The prepreg according to any one of claims 1 to 3, wherein the surface heating treatment in step 3 is a treatment of heating the prepreg precursor in an environment of 200 to 700 ° C. 如請求項1至4中任一項所述之預浸體，其中，步驟3中的表面加熱處理的加熱時間為1.0～10.0秒。The prepreg according to any one of claims 1 to 4, wherein the heating time of the surface heating treatment in step 3 is 1.0 to 10.0 seconds. 如請求項1至5中任一項所述之預浸體，其中，前述基材為玻璃布。The prepreg according to any one of claims 1 to 5, wherein the substrate is glass cloth. 一種積層板，其是將請求項1至6中任一項所述之預浸體與金屬箔積層並進行成形而成。A laminated board obtained by laminating and forming the prepreg and metal foil according to any one of claims 1 to 6. 一種印刷線路板，其是包含請求項1至6中任一項所述之預浸體或請求項7所述之積層板而成。A printed wiring board comprising a prepreg according to any one of claims 1 to 6 or a laminated board according to claim 7. 一種半導體封裝體，其是使用請求項8所述之印刷線路板而成。A semiconductor package using the printed wiring board according to claim 8. 一種預浸體的製造方法，其是用以製造請求項1至6中任一項所述之預浸體的方法，並且，具有下述步驟1～3： 　　步驟1：獲得預浸體前驅物的步驟，並且，前述預浸體前驅物是對熱硬化性樹脂組成物進行B階段化而成，且於前述B階段化中，使熱硬化性樹脂組成物含浸於基材中之後實施加熱處理； 　　步驟2：將步驟1中獲得的預浸體前驅物冷卻的步驟； 　　步驟3：獲得預浸體的步驟，並且，前述預浸體是對在步驟2中冷卻後的預浸體前驅物實施表面加熱處理來獲得，且前述表面加熱處理是使預浸體前驅物的表面溫度上升的處理。A method for manufacturing a prepreg, which is a method for manufacturing the prepreg according to any one of claims 1 to 6, and has the following steps 1 to 3: Step 1: Obtaining a prepreg precursor In addition, the prepreg precursor is obtained by subjecting the thermosetting resin composition to a B-stage process, and in the B stage, the thermosetting resin composition is impregnated into a substrate and then subjected to a heat treatment. Step 2: The step of cooling the prepreg precursor obtained in Step 1; Step 3: The step of obtaining a prepreg, and the aforementioned prepreg is implemented on the prepreg precursor cooled in Step 2 It is obtained by surface heating treatment, and the aforementioned surface heating treatment is a treatment for raising the surface temperature of the prepreg precursor.
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