567139 A7 __ _ B7 五、發明説明（彳） 【發明所屬之技術領域】 (請先閲讀背面之注意事項再填寫本頁) 本發明係關於保持環氧樹脂組成物於玻璃纖維織布母 材的表面層；及保持至少含有氫氧化鋁作爲無機塡充材之 環氧樹脂組成物於玻璃纖維不織布母材的中央層，利用力口 熱加壓成形而一體化之合成疊層板及此合成疊層板的製造 方法之發明。 【先行技術】 上述合成疊層板係廣泛地被使用作爲在表面層上接合 銅箔等而構成的印刷電路板之絕緣層，中央層的氫氧化鋁 是以給予不燃性於合成疊層板爲目的而混合於環氧樹脂組 成物中。氫氧化鋁係在高溫（2 0 0 °C左右）開始熱分解 ，產生水蒸氣而發揮不燃效果。 經濟部智慧財產局員工消費合作社印製 可是當氫氧化鋁的熱分解溫度低時，就會使疊層板的 耐熱性（銲錫耐熱性）下降。氫氧化鋁的熱分解開始溫度 係由氫氧化鋁之製造條件而不同。使使用的氫氧化鋁中之 氧化鈉的含有率越少，熱分解開始溫度會變越高。在於工 業用氫氧化鋁，氫氧化鋁中之氧化鈉含有率成爲熱耐性之 指數。在高耐熱用途的工業用氫氧化鋁，氧化鈉含有率是 被管理於大約0 · 1質量％以下。 在印刷電路板製造用的合成疊層板所要求之銲錫耐熱 性係在以J I S所定之基準，使合成疊層板的板測試片浮 於2 6 0 °C的銲錫浴中，經過2 0秒以上在疊層板不會發 生異常之事。可是在實際上，因考慮安全率等，以經過 本紙張尺度適用中國國家標準（CNS ) A4規格（210X297公釐） -4- 567139 A7 B7 五、發明説明（2) 1 2 0秒以上在疊層板上不會發生異常來作爲基準。 (請先閲讀背面之注意事項再填寫本頁) 從此種狀況，採用高耐熱用途的氫氧化鋁作爲混合於 使用在合成疊層板的中央層中的環氧樹脂組成物之氫氧化 鋁。特別是使用在中央層之環氧樹脂組成物中，使其含有 3 0質量％以上之氫氧化銘的情況時，是必需使用高耐熱 用途之氫氧化鋁。如果在此種條件之情況下，採用氧化鈉 含有率超過0 · 1質量％的一般用途用之氫氧化鋁的時， 在經過前述的1 2 0秒之前，在疊層板上就會發生異常。 【發明所欲解決之課題】 經濟部智慧財產局員工消费合作社印製 本發明之所欲解決之課題係提昇使用於中央層之環氧 樹脂組成物中至少含有氫氧化鋁作爲無機塡充材料的合成 疊層板之銲錫耐熱性之事。且本發明之所欲解決之課題係 在使用限制含有不純物氧化鈉的量之高耐熱用途的氫氧化 鋁時，更能提昇採用相同的氫氧化鋁之以往的合成疊層板 之銲錫耐熱性之事。又本發明之所欲解決之課題係即使使 用增加含有不純物氧化鈉的量之一般用途用之氫氧化鋁時 ，也能接近使用高耐熱用途的以往的合成疊層板之銲錫耐 熱性之事。 【用以解決課題之手段】 本發明係在疊層保持環氧樹脂組成物於玻璃纖維織布 母材的表面層，及保持至少含有氫氧化鋁作爲無機塡充材 料之環氧樹脂組成物於玻璃纖維不織布母材的中央層之狀 本紙張尺度適用中國國家標準（CNS ) A4規格（210X297公釐） -5- 567139 A7 B7 _ 五、發明説明（3) (請先閱讀背面之注意事項再填寫本頁) 態下，利用加熱加壓成形而一體化之合成疊層板作爲改良 之對象。以更具體的標準來說明的話，本發明係疊層浸漬 第1環氧樹脂組成物在玻璃纖維織布母材上，加熱乾燥之 表面層聚脂膠片，及浸漬至少含有氫氧化鋁作爲無機塡充 材料的第2環氧樹脂組成物在玻璃纖維不織布母材上，加 熱乾燥之中央層聚脂膠片，這些預浸料受到加熱加壓成形 而一體化，由硬化的表面層聚脂膠片來構成表面層，由硬 化的中央層聚脂膠片來構成中央層之合成疊層板作爲改良 之對象。 經濟部智慧財產局員工消費合作社印製 在本發明之合成疊層板，在加熱加壓成形時，表面層 中的環氧樹脂組成物與保持於表面層中之環氧樹脂組成物 呈相連接之狀態下，延伸至中央層之內部，在中央層中形 成複數個樹脂集中處，這些複數個樹脂集中處發生硬化而 構成複數個固定部。以更具體的標準來看，中央層係具有 可使溶融樹脂流入的複數個空隙。且被浸漬在表面層聚脂 膠片的第1環氧樹脂組成物的一部份進入中央層聚脂膠片 的複數個空隙，形成複數個樹脂集中處，這些複數個樹脂 集中處在與表面層中的第1環氧樹脂組成物相連之狀態下 硬化，形成提高表面層與中央層之機械的結合強度之複數 個固定部。 根據本發明的合成疊層板的話，利用複數個樹脂集中 處硬化而形成複數個固定部的存在，增加表面層與中央層 的黏合面積。且利用固定部之固定效果或楔入效果（固定 部係呈深入中央層之狀態，卡合於中央層之效果）增大表 本紙張尺度適用中國國家標準（CNS ) A4規格（210X297公釐） " -6- 經濟部智慧財產局員工消費合作社印製 567139 A7 B7 五、發明説明（J ^^ 47 面層與中央層之間的層間接著強度。由於這些結果，即使 在中央層中的氫氧化鋁發生熱分解而產生水蒸氣之情況下 ’也不易產生表面層與中央層之間的層間剝離，且能提昇 耐熱性。 再者即使固定部的尺寸小，也能夠得到固定效果。可 是在實用上，其最大尺寸（不問位置及方向，在能測定的 尺寸中之最大尺寸）係1 0 0 //rn以上較佳。再者固定部 係只要有一個的話就能得到固定效果。可是在實用上，在 平均1 0 0cm2中，存在有1 〇 〇個〜2 0 0個的固定部較 佳。因此，在中央層聚脂膠片上，在平均1 〇 〇 cm 2中，必 需存在有1 00//m以上的空隙2 0 0個〜40 0個。 爲了得到良好之固定部，使用加熱乾燥後的被浸漬之 第1環氧樹脂組成物的加熱加壓成形時的最低溶融黏度成 爲5 0〜5 0 0 P a · s (帕斯卡秒）之物品來作爲表面 層聚脂膠片；使用加熱乾燥後的被浸漬之第2環氧樹脂組 成物的最低溶融黏度較在加熱加壓成形時的表面層聚脂膠 片中的第1環氧樹脂組成物的最低溶融黏度爲大之物品來 作爲中央層聚脂膠片爲較佳。能夠使用加熱乾燥後的被浸 漬之第2環氧樹脂組成物的加熱加壓成形時之最低溶融黏 度成爲0 · 01〜0 · 05MPa · s之物品作爲具體的 中央層聚脂膠片。 在製造本發明之合成疊層板時，浸漬第1環氧樹脂組 成物於玻璃纖維織布母材，製造加熱乾燥後之表面層聚脂 膠片。當製造表面層聚脂膠片時，進行加熱乾燥，使在浸 本紙張尺度適用中國國家標準（CNS ) A4規格（210X297公董1 (請先閲讀背面之注意事項再填寫本頁)567139 A7 __ _ B7 V. Description of the invention (彳) [Technical field to which the invention belongs] (Please read the precautions on the back before filling out this page) This invention is about maintaining the epoxy resin composition in the glass fiber woven base material. A surface layer; and a synthetic laminated board which holds an epoxy resin composition containing at least aluminum hydroxide as an inorganic concrete filling material in a central layer of a glass fiber non-woven base material, and is integrated by thermocompression molding, and the synthetic laminate Invention of a method for manufacturing a laminate. [Preceding technology] The above-mentioned synthetic laminated board is widely used as an insulating layer of a printed circuit board formed by bonding copper foil or the like to a surface layer. The aluminum hydroxide in the center layer is used to give noncombustibility to the synthetic laminated board. It is mixed with an epoxy resin composition for the purpose. Aluminum hydroxide system starts thermal decomposition at high temperature (about 200 ° C), generates water vapor and exerts non-combustible effect. Printed by the Consumer Cooperative of the Intellectual Property Bureau of the Ministry of Economic Affairs. However, when the thermal decomposition temperature of aluminum hydroxide is low, the heat resistance (solder heat resistance) of the laminated board is reduced. The thermal decomposition starting temperature of aluminum hydroxide differs depending on the production conditions of aluminum hydroxide. The lower the content of sodium oxide in the used aluminum hydroxide, the higher the thermal decomposition onset temperature. Because industrial hydroxide is used, the content of sodium oxide in aluminum hydroxide becomes an index of thermal resistance. For industrial aluminum hydroxide with high heat resistance, the content of sodium oxide is controlled to about 0.1% by mass or less. The required solder heat resistance of the synthetic laminated board for printed circuit board manufacturing is to float the board test piece of the synthetic laminated board in a solder bath at 260 ° C in accordance with the JIS standard for 20 seconds. The above does not cause any abnormality in the laminated board. However, in practice, due to the consideration of safety factors, etc., the Chinese National Standard (CNS) A4 specification (210X297 mm) is applied after passing through this paper scale. 567 139139 A7 B7 V. Description of the invention (2) Over 1 2 0 seconds No abnormality will occur on the shelf as a reference. (Please read the notes on the back before filling this page.) From this situation, aluminum hydroxide with high heat resistance is used as the aluminum hydroxide mixed with the epoxy resin composition used in the center layer of the synthetic laminate. In particular, when the epoxy resin composition used in the center layer contains 30% by mass or more of hydroxide hydroxide, it is necessary to use aluminum hydroxide with high heat resistance. Under these conditions, when using aluminum hydroxide for general purpose with a sodium oxide content exceeding 0.1% by mass, an abnormality may occur on the laminated board before the aforementioned 120 seconds elapse. . [Problems to be Solved by the Invention] The Consumer Cooperatives of the Intellectual Property Bureau of the Ministry of Economic Affairs printed the problem to be solved by the present invention is to promote the use of epoxy resin compositions in the central layer that contain at least aluminum hydroxide as an inorganic filler. The matter of solder heat resistance of synthetic laminated board. Moreover, the problem to be solved by the present invention is to improve the solder heat resistance of conventional synthetic laminates using the same aluminum hydroxide when using aluminum hydroxide with high heat resistance for which the amount of impurities containing sodium oxide is used. thing. The problem to be solved by the present invention is that even when aluminum hydroxide for general use containing an increased amount of impurity sodium oxide is used, it is possible to approach the solder heat resistance of a conventional synthetic laminated board using high heat resistance. [Means to solve the problem] The present invention is to maintain an epoxy resin composition on a surface layer of a glass fiber woven base material in a laminate, and to hold an epoxy resin composition containing at least aluminum hydroxide as an inorganic filler material. The shape of the central layer of the glass fiber non-woven base material This paper applies the Chinese national standard (CNS) A4 specification (210X297 mm) -5- 567139 A7 B7 _ 5. Description of the invention (3) (Please read the precautions on the back before (Fill in this page) In the state, the integrated laminated board integrated by heating and pressure forming is the object of improvement. To explain by more specific standards, the present invention is based on laminating and impregnating a first epoxy resin composition on a glass fiber woven base material, heating and drying a surface layer of polyester film, and impregnating at least aluminum hydroxide as an inorganic hafnium The second epoxy resin composition of the filling material is a glass fiber non-woven base material, and the central layer of polyester film is heated and dried. These prepregs are heated and press-molded and integrated, and are composed of a hardened surface layer of polyester film. As the surface layer, a composite laminated plate composed of a cured central layer polyester film as the central layer is the object of improvement. The consumer cooperative of the Intellectual Property Bureau of the Ministry of Economic Affairs printed the synthetic laminated board of the present invention. During the heating and pressure forming, the epoxy resin composition in the surface layer and the epoxy resin composition held in the surface layer are connected. In this state, it extends to the inside of the center layer, and a plurality of resin concentrations are formed in the center layer. These resin concentrations are hardened to form a plurality of fixing portions. By more specific standards, the central layer has a plurality of voids through which molten resin can flow. And a part of the first epoxy resin composition impregnated in the surface layer polyester film enters a plurality of voids in the center layer polyester film to form a plurality of resin concentrations, and these plurality of resin concentrations are in the surface layer. The first epoxy resin composition is hardened in a connected state to form a plurality of fixing portions that increase the mechanical bonding strength of the surface layer and the central layer. According to the synthetic laminated board of the present invention, the existence of a plurality of fixing portions is formed by curing a plurality of resin concentrations, thereby increasing the bonding area between the surface layer and the center layer. And use the fixed effect or wedge effect of the fixed part (the fixed part is in the state of the central layer, the effect of engaging in the central layer) to increase the paper size of the paper to apply the Chinese National Standard (CNS) A4 specification (210X297 mm) " -6- Printed by the Consumer Cooperatives of the Intellectual Property Bureau of the Ministry of Economic Affairs 567139 A7 B7 V. Description of the invention (J ^ 47 47 The layer between the surface layer and the central layer is indirect strength. Due to these results, even the hydrogen in the central layer When alumina is thermally decomposed to generate water vapor, it is not easy to cause interlayer peeling between the surface layer and the center layer, and it can improve heat resistance. Moreover, even if the size of the fixed portion is small, a fixing effect can be obtained. Practically, the maximum size (the largest size among the measurable sizes regardless of position and direction) is preferably 1 0 0 // rn or more. Moreover, if there is only one fixing part, the fixing effect can be obtained. Practically, it is preferable that there are 100 to 200 fixing parts in an average of 100 cm2. Therefore, in the central layer polyester film, in an average of 100 cm2, it is necessary Between 200 and 400, where there are gaps of 100 // m or more. In order to obtain a good fixing part, the lowest melting point during heating and pressure molding using the first epoxy resin composition impregnated after heating and drying is used. Articles with a viscosity of 50 to 500 Pa (s Pascal seconds) are used as the surface layer polyester film; the lowest melt viscosity of the second epoxy resin composition impregnated after heating and drying is higher than that under heat and pressure The first epoxy resin composition in the surface layer polyester film at the time of molding is preferably the one having the largest melt viscosity as the center layer polyester film. The second epoxy resin impregnated after heating and drying can be used. When the composition has a minimum melt viscosity of 0 · 01 ~ 0 · 05MPa · s when the composition is heated and pressed, it is used as a concrete central polyester film. When manufacturing the synthetic laminate of the present invention, the first epoxy resin is impregnated. The composition is made of glass fiber woven base material, and the surface layer polyester film after heating and drying is manufactured. When the surface layer polyester film is manufactured, it is heated and dried, so that the Chinese national standard (CNS) A4 specification is applied to the paper size. 210 X297 公 董 1 (Please read the notes on the back before filling this page)
567139 A7 B7 五、發明説明（5) 漬於玻璃纖維織布母材的第1環氧樹脂組成物的加熱加壓 成形時的最低溶融黏度成爲5 0〜5 0 0 P a · S。再者 製造浸漬至少含有氫氧化鋁作爲無機塡充材料之第2環氧 樹脂組成物於玻璃纖維不織布母材，加熱乾燥後的中央層 聚脂膠片。在製造中央層聚脂膠片時，在合成疊層板的加 熱加壓成形時留下能夠使溶融樹脂流入的複數個空隙，且 加熱乾燥使浸漬於玻璃纖維不織布的環氧樹脂組成物的最 低溶融黏度較在加熱加壓成形時的表面層聚脂膠片中的第 1環氧樹脂組成物的最低溶融黏度大。再加上在疊層表面 層聚脂膠片與中央層聚脂膠片的狀態下，加熱加壓成形使 兩者一體化，由硬化後的表面層聚脂膠片形成表面層，由 硬化後的中央層聚脂膠片形成中央層。在於本發明，在加 熱加壓成形時，使被浸漬於表面層聚脂膠片之第1環氧樹 脂組成物的一部份進入中央層聚脂膠片中的複數個空隙， 形成複數個樹脂集中處，在與表面層聚脂膠片中之第1環 氧樹脂組成物相連接之狀態下使這些複數個樹脂集中處硬 化。 如上述般之製造成的合成疊層板係因在表面層聚脂膠 片中之第1環氧樹脂組成物的加熱加壓成形時之最低溶融 黏度低，在中央層聚脂膠片中的第2環氧樹脂組成物溶融 且塡滿空隙之前，流入殘留於中央層聚脂膠片中的空隙中 形成樹脂集中處。此樹脂集中處係與表面層聚脂膠片中之 第1環氧樹脂組成物呈相連接之狀態下延伸至中央層內部 ，分布於中央層中，硬化後成爲固定部。且，因表面層聚 本纸張尺度適用中國國家標準（CNS ) A4規格（210 X297公董1 ^ -8- (請先閲讀背面之注意事項再填寫本頁) 裝·567139 A7 B7 V. Description of the invention (5) The minimum melt viscosity of the first epoxy resin composition stained on the glass fiber woven base material during heating and pressing becomes 50 to 5 0 P a · S. Furthermore, a second-layer epoxy resin sheet was prepared by impregnating a second epoxy resin composition containing at least aluminum hydroxide as an inorganic filler into a glass fiber nonwoven fabric base material and heating and drying it. In the manufacture of the central layer polyester film, a plurality of voids capable of allowing the molten resin to flow in are left during the heat and pressure molding of the synthetic laminated board, and the heating and drying are performed to minimize the melting of the epoxy resin composition impregnated with the glass fiber nonwoven fabric. The viscosity is greater than the lowest melt viscosity of the first epoxy resin composition in the surface layer polyester film during heat and pressure molding. In addition, in a state where the surface layer polyester film and the center layer polyester film are laminated, the two layers are integrated by heating and pressure forming. The surface layer is formed by the cured surface layer polyester film, and the core layer after curing is formed. The polyester film forms the central layer. In the present invention, during the heat and pressure molding, a part of the first epoxy resin composition immersed in the surface layer polyester film is allowed to enter a plurality of voids in the center layer polyester film to form a plurality of resin concentrations. The plurality of resin concentrates are hardened while being connected to the first epoxy resin composition in the surface layer polyester film. The synthetic laminated board manufactured as described above has the lowest melt viscosity during heating and pressure molding of the first epoxy resin composition in the surface layer polyester film, and the second epoxy resin composition in the center layer polyester film has the lowest melt viscosity. Before the epoxy resin composition is melted and filled with voids, it flows into the voids remaining in the polyester film in the center layer to form a resin concentration. This resin concentration point is connected to the first epoxy resin composition in the surface layer polyester film and extends to the inside of the center layer, is distributed in the center layer, and becomes a fixed part after curing. In addition, because the surface layer is aggregated, this paper is sized to the Chinese National Standard (CNS) A4 specification (210 X297 Public Manager 1 ^ -8- (Please read the precautions on the back before filling out this page).
、1T 經濟部智慧財產局員工消費合作社印製 經濟部智慧財產局員工消资合作社印製 567139 A7 ____B7 五、發明説明（6) 脂膠片中的第1環氧樹脂組成物之最低溶融黏度較前述之 値更低時就會使疊層板之厚度的精準度調節變困難，又較 前述之値更高時就會無法形成良好之樹脂集中處，所以使 用上述的數値範圍之物品爲最合適。再者中央層聚脂膠片 中的第2環氧樹脂組成物之最低溶融黏度較前述之値（ 〇·〇1〜〇· 0 5 Μ P a · S )更低時空隙會被第2環 氧樹脂所塡埋。又較前述之値爲更高時就會因第2環氧樹 脂的流動不足，易發生浸透不足之現象。 【發明之實施型態】 在於本發明，能夠採用含有超過〇 · 1質量％的不純 物氧化鈉之一般用途的氫氧化鋁，即使在該情況下，與採 用以往的高耐熱用途之氫氧化鋁時相同，可確保合成疊層 板之銲錫耐熱性。因能夠採用一般用途之氫氧化銘之事， 所以可謀求減低材料成本。不過，氫氧化鋁中之氧化鈉含 有量係管理於0 · 2質量％以下較佳。當然，在於本發明 ，採用高耐熱用途之氫氧化鋁就會使同樣採用高耐熱用途 之氫氧化鋁的以往之合成疊層板的銲錫耐熱性更爲提高。 在中央層的第2環氧樹脂組成物，除了氫氧化鋁作爲 無機塡充材料之外，通常被使用之無機塡充材料亦可與例 如滑石一同混合。第2環氧樹脂組成物中的氫氧化鋁含有 率係從賦予不燃性與確保耐熱性的觀點來看，管理於2 0 〜4 0質量％爲最合適。 如上述般，將環氧樹脂浸漬於玻璃纖維織布母材，乾 ^紙張尺度適用中國國家標準（CNS)八4祕（210x297公董） ' ' -9 - (請先閱讀背面之注意事項再填寫本頁)、 1T printed by the Consumer Cooperative of Intellectual Property Bureau of the Ministry of Economic Affairs and printed by employees of the Intellectual Property Bureau of the Ministry of Economic Affairs and printed by employees of the Intellectual Property Bureau of the Ministry of Economic Affairs 567139 A7 ____B7 V. Description of the invention (6) The lowest melting viscosity of the first epoxy resin composition in the fat film is higher than the foregoing When it is lower, it will be difficult to adjust the thickness of the laminated board, and when it is higher than the above, it will not be able to form a good resin concentration. Therefore, it is most suitable to use the above range. . Furthermore, when the lowest melting viscosity of the second epoxy resin composition in the polyester film of the central layer is lower than the aforementioned 前述 (〇 · 〇1〜〇 · 0 5 Μ P a · S), the void will be affected by the second epoxy. Resin buried. If it is higher than the above, the second epoxy resin is insufficient in flow, and the phenomenon of insufficient penetration is likely to occur. [Embodiment of the invention] In the present invention, it is possible to use general purpose aluminum hydroxide containing more than 0.1% by mass of impure sodium oxide, and even in this case, when using conventional aluminum hydroxide with high heat resistance, Also, the solder heat resistance of the composite laminated board can be ensured. Since the general purpose hydroxide name can be used, material cost can be reduced. However, it is preferable that the content of sodium oxide in aluminum hydroxide is controlled to 0.2% by mass or less. Of course, in the present invention, the use of aluminum hydroxide having a high heat resistance makes it possible to further improve the solder heat resistance of a conventional synthetic laminated board which also uses aluminum hydroxide having a high heat resistance. The second epoxy resin composition in the center layer can be mixed with, for example, talc, in addition to aluminum hydroxide, as the inorganic filler. The content of the aluminum hydroxide in the second epoxy resin composition is most preferably controlled from 20 to 40% by mass from the viewpoint of imparting incombustibility and securing heat resistance. As mentioned above, the epoxy resin is impregnated with the glass fiber woven base material, and the paper size of the paper is applicable to China National Standards (CNS) Eighty-fourth Secretary (210x297). '' -9-(Please read the precautions on the back before (Fill in this page)
567139 經濟部智慧財產局員工消費合作社印製 A7 _B7_五、發明説明（7) 燥加熱來製造之表面層聚脂膠片係調整製造合成疊層板的 加熱加壓成形的樹脂的最低溶溶黏度於5 0〜5 0 0 P a • s 。另一方面，雖設定中央層聚脂膠片的樹脂的最低溶 融黏度較表面層聚脂膠片的樹脂的最低溶融黏度高，不過 其最低溶融黏度係調整在0 · 0 1〜0 · 0 5 Μ P a · s 的範圍內爲最合適。這些最低溶融黏度的調整係利用變換 製造預浸料時的加熱乾燥程度來實施。 在合成疊層板的加熱加壓成形時，因使第1環氧樹脂 組成物的溶融樹脂流入中央層聚脂膠片的空隙中，中央層 聚脂膠片中的樹脂含有量（包含無機塡充材料於含有量中 )係成爲9 5質量％以下來進行環氧樹脂組成物朝向玻璃 纖維不織布母材的浸漬爲佳。 利用標準的合成疊層板製造方法來製造上述般的表面 層聚脂膠片與中央層聚脂膠片。 【實施例】 以下，關於本發明之實施例1〜5，說明關於比較例 1以及以住例1與2。 利用將不含無機塡充材料的溴化環氧樹脂作爲主體之 第1環氧樹脂組成物浸漬於玻璃纖維織布母材加熱乾燥， 製造B階段的表面層聚脂膠片。使用的玻璃纖維織布母材 係纖維是9 // m，將此纖維收集成束作成之線的直徑是 0 · 1 6 nun，使用此線的織布之編織密度是在2 5腿寬幅 中縱4 4條、橫3 2條，厚度是0 · 2 mm的平織玻璃纖維 本紙張尺度適用中國國家標準（CNS ) A4規格（210X297公釐） 義10- (請先閱讀背面之注意事項再填寫本頁) .裝· 訂 線 567139 A7 B7 五、發明説明（8) (請先閲讀背面之注意事項再填寫本頁) 織布。表面層聚脂膠片的樹脂含有量係控制在4 5質量％ 。在實施例使用之物品，利用變換乾燥溫度（1 7 〇 °C以 下）及/或乾燥時間的設定’來調整B階段的樹脂的硬化 度，使之後在加熱加壓成形時的樹脂組成物之最低溶融黏 度變成5〇〜5〇〇Pa · s 。 再者，利用將含有3 0質量％的氫氧化銘、2 7質量 %的滑石作爲無機塡充材料的溴化環氧樹脂來作爲主體之 第2環氧樹脂組成物浸漬於玻璃纖維不織布母材乾燥加熱 ，製造B階段的中央層聚脂膠片。製造中央層聚脂膠片的 (含有無機塡充材料的樹脂含有量9 0質量％ )。使用被 製造爲使用粗1 0 A m、長度8腿的玻璃纖維’成爲單位 質量9 0 g ./ m 2、厚0 · 7 mm之物品作爲玻璃纖維不織布 母材。在1 7 0 °C以下的溫度來進行加熱乾燥’使之後的 再加熱加壓成形時的樹脂組成物之最低溶融黏度成爲 〇.〇3MPa · s。如此形成之中央層聚脂膠片係具有 在平均1 0 0cm2上，形成如1 0 0 以上的2 5 0個〜 3 5 0個之後述的樹脂集中處或固定部的空隙。 經濟部智慧財產局員工消費合作社印製 將上述的中央層聚脂膠片重疊成對折，在其兩面上重 疊各一片的上述之表面層聚脂膠片，且將3 5 //m厚的銅 箔載置於表面層聚脂膠片之上，利用將這些加熱加壓成形 之事，作成板厚1 · 6 nim的合成疊層板。此時之加熱溫度 是1 7 5°C、壓力是8MP a、加熱時間是6 0分鐘。 在實施例、比較例、以往例’在使用後的表面層聚脂 膠片之加熱加壓成形時之第1環氧樹脂組成物的最低溶融 本紙張尺度適用中國國家標準（CNS ) A4規格（210X297公董Ί -11 - 567139 經濟部智慧財產局員工消費合作社印製 五、發明説明（9) 黏度係同表1所示。中央層聚脂膠片的加熱加壓成形時的 最低溶融黏度不管任何一例皆爲0 . 0 3 Μ P a · s。且 在各例包含於第2環氧樹脂組成物的氫氧化鋁的不純物之 氧化鈉的含有量係同表1所示。 【表1】 表面層聚脂膠片 樹脂最低溶融黏度 (Pa · s) A1(〇H)3中之Na2〇 量 (質量％) 樹脂集中處 最大尺寸 (β m) 銲錫耐熱性 (秒） 實施例1 100 004 280 300以上 實施例2 50 016 410 300以上 實施例3 100 016 280 280 實施例4 300 016 140 220 實施例5 500 016 100 200 比較例1 1000 016 無(小尺寸•少數) 110 以往例1 2000 004 並 j \ w 252 以往例2 2000 016 並 jw\ 92 關於上述各例的合成疊層板，觀察其剖面。第1圖係 以模式表示之實施例的合成疊層板之剖面圖。表面層樹脂 係從表面層1到達至中央層2 ，在中央層中形成樹脂集中 處3。此樹脂集中處硬化而構成固定部。樹脂集中處（或 固定部）3係多數地分布於中央層中。相對於比較例1的 本紙張尺度適用中國國家標準（CNS ) A4規格（210 X 297公釐） (請先閱讀背面之注意事項再填寫本頁)567139 Printed by the Consumer Cooperative of the Intellectual Property Bureau of the Ministry of Economic Affairs A7 _B7_ V. Description of the Invention (7) The surface layer polyester film produced by drying and heating is adjusted to the minimum melt viscosity of the resin produced by heat and pressure forming of synthetic laminate 5 0 ~ 5 0 0 P a • s. On the other hand, although the minimum melt viscosity of the resin of the central layer polyester film is set higher than the minimum melt viscosity of the resin of the surface layer polyester film, the minimum melt viscosity is adjusted to 0 · 0 1 ~ 0 · 0 5 Μ P The most appropriate range is a · s. These minimum melt viscosity adjustments are performed by changing the degree of heat drying during the manufacture of the prepreg. During the heat and pressure molding of the synthetic laminate, the molten resin of the first epoxy resin composition flows into the gap of the central layer polyester film, and the resin content in the central layer polyester film (including the inorganic filler material) In the content), it is preferably 95% by mass or less to impregnate the epoxy resin composition toward the glass fiber nonwoven fabric base material. The above-mentioned surface layer polyester film and center layer polyester film are manufactured by a standard synthetic laminate manufacturing method. [Examples] Hereinafter, Examples 1 to 5 of the present invention will be described with respect to Comparative Example 1 and Living Examples 1 and 2. A first epoxy resin composition containing a brominated epoxy resin containing no inorganic filler as a main body was immersed in a glass fiber woven fabric base material and dried by heating to produce a surface layer polyester film in the B stage. The fiberglass woven base material fiber used is 9 // m. The diameter of the thread collected from this fiber into a bundle is 0 · 1 6 nun. The weaving density of the woven fabric using this thread is 2 5 legs wide. Flat woven glass fiber with 4 4 in the middle and 3 2 in the horizontal, and a thickness of 0 · 2 mm. The paper size is applicable to the Chinese National Standard (CNS) A4 specification (210X297 mm). Meaning 10- (Please read the precautions on the back first. Fill out this page). Binding and Thread 567139 A7 B7 V. Description of the invention (8) (Please read the precautions on the back before filling this page) Weaving. The resin content of the surface layer polyester film is controlled to 45 mass%. In the articles used in the examples, the drying temperature (1700 ° C or lower) and / or the setting of the drying time are used to adjust the hardening degree of the B-stage resin, so that the resin composition in the subsequent heating and pressure molding can be adjusted. The minimum melting viscosity becomes 50 to 500 Pa · s. Furthermore, a glass epoxy nonwoven fabric base material was impregnated with a second epoxy resin composition as a main body by using a brominated epoxy resin containing 30% by mass of hydroxide hydroxide and 27% by mass of talc as an inorganic filler. Drying and heating to produce a central layer polyester film in the B stage. Production of a central layer polyester film (90% by mass of resin content containing inorganic filler). A glass fiber made of a thickness of 10 A m and a length of 8 legs was used as a unit weight of 90 g ./ m 2 and a thickness of 0 · 7 mm as a glass fiber non-woven base material. The heating and drying are performed at a temperature of 170 ° C or lower 'so that the minimum melt viscosity of the resin composition at the time of the subsequent reheating and pressing molding is 0.03 MPa · s. The thus-formed central layer polyester film has voids at a resin concentration or fixing portion of 250 to 350 as described later, such as 100 or more, on an average of 100 cm2. Printed by the Consumer Cooperative of the Intellectual Property Bureau of the Ministry of Economic Affairs, the above-mentioned central layer of polyester film is folded into two, and one piece of the above-mentioned surface layer of polyester film is overlapped on both sides, and a copper foil of 3 5 // m thickness is loaded. It was placed on the surface layer of the polyester film, and a composite laminated board having a thickness of 1 · 6 nim was formed by using these heat and pressure molding. The heating temperature at this time was 175 ° C, the pressure was 8MP a, and the heating time was 60 minutes. In the Examples, Comparative Examples, and Conventional Examples, the minimum melting point of the first epoxy resin composition when the surface layer polyester film is heated and press-formed after use. The paper size applies the Chinese National Standard (CNS) A4 specification (210X297). Gong Dongyu -11-567139 Printed by the Consumer Cooperatives of the Intellectual Property Bureau of the Ministry of Economic Affairs 5. Description of the invention (9) The viscosity is the same as shown in Table 1. The minimum melt viscosity of the central layer polyester film during heat and pressure molding does not matter any case All are 0.03 MPa · s. The content of sodium oxide in the impurities of the aluminum hydroxide contained in the second epoxy resin composition in each example is as shown in Table 1. [Table 1] Surface layer Polyester film resin minimum melting viscosity (Pa · s) Na2O content (mass%) in A1 (〇H) 3 Maximum size of resin concentration (β m) Solder heat resistance (seconds) Example 1 100 004 280 300 or more Example 2 50 016 410 300 or more Example 3 100 016 280 280 Example 4 300 016 140 220 Example 5 500 016 100 200 Comparative Example 1 1000 016 None (small size • few) 110 Conventional Example 1 2000 004 and j \ w 252 Conventional example 2 2000 016 and jw \ 92 Regarding the composite laminates of the above examples, observe the cross-sections. Fig. 1 is a cross-sectional view of the composite laminates of the embodiment shown in a pattern. The surface layer resin reaches from the surface layer 1 to the center layer 2, and at the center layer A resin concentration point 3 is formed in the resin. This resin concentration point is hardened to form a fixed portion. The resin concentration point (or fixed portion) 3 is mostly distributed in the central layer. Compared to the paper size of Comparative Example 1, the Chinese national standard (CNS) is applied. ) A4 size (210 X 297 mm) (Please read the notes on the back before filling this page)
Γ -12- 567139 A7 _____B7 五、發明説明（^ 合成疊層板即使形成樹脂集中處也不顯著，在以往例1 2的合成疊層板沒有形成樹脂集中處。在表1 ，一倂表示 (請先閱讀背面之注意事項再填寫本頁) 幵< 成的樹脂集中處3之最大尺寸與銲錫耐熱性測定結果。 表中，表面層聚脂膠片的最低溶融黏度係以高架式流 動測試器（昇溫速度2 °C /分）來測定。 樹脂集中處的尺寸最大値係在測試片的剖面觀察長度 1 0 cm中看到的樹脂集中處硬化而形成固定部的最大尺寸 0 銲錫耐熱性係根據J I S - C 5 0 1 3，測定將測試 片放在溶融銲錫（2 6 0 °C )上，在測試片表面發生氣泡 爲止的時間之耐熱性（η = 5之平均値）。 再者雖然在表1無表示，不過在各實施例，在中央層 中，平均1 0 Ocm 2中形成1 2 0個〜1 8 0個的樹脂集中 處（固定部）。 經濟部智慧財產局員工消費合作社印製 從表1來能淸楚地了解，在關於本發明的各實施例， 形成良好的樹脂集中處（固定部），具有優良的銲錫耐熱 性。其次觀看實施例2〜5能了解到即使使用包含有超過 〇· 1質量％、含有0 · 1 6質量％的不純物氧化鈉之氫 氧化鋁的第2環氧樹脂組成物時，亦可得到良好之銲錫耐 熱性。且使用含有高耐熱用途的氫氧化鋁（含有未滿 〇· 1質量％之不純物氧化鈉者）之第2環氧樹脂組成物 於中央層聚脂膠片之實施例1 ，與採用相同的高耐熱用途 的氫氧化鋁之以往例1相比較就能明瞭在實施例1中的銲 錫耐熱性較以往例1更能向上提高。 本紙張尺度適用中國國家標率（CNS ) A4規格（210X297公釐） -13 - 567139 A7 B7 五、發明説明（j 【發明效果】 如上述般，關於本發明之合成疊層板係在中央層的環 氧樹脂組成物中，雖含有氫氧化鋁作爲無機塡充材料，不 過因在表面層中的環氧樹脂組成物是與表面層成相連之狀 態下延伸至中央層，構成分布於中央層中的樹脂集中處（ 固定部），所以耐熱性是優良的。且關於本發明之方法係 對於製造前述結構的合成疊層板爲有效的方法。 【圖面之簡單說明】 第1圖係以模式表示關於本發明實施例的合成疊層板 的剖面說明圖。 【圖號說明】 1 :表面層 2 :中央層 3 :樹脂集中處（固定部） (請先閲讀背面之注意事項再填寫本頁) 經濟部智慧財產局員工消費合作社印製 本紙張尺度適用中國國家標準（CNS ) A4規格（210X297公釐） •14-Γ -12- 567139 A7 _____B7 V. Description of the invention (^ Synthetic laminates are not significant even if they form a resin concentration point. In the conventional example 12, the synthetic laminates did not form a resin concentration point. In Table 1, it is indicated by () (Please read the precautions on the back before filling in this page) 幵 < the maximum size of the resin concentration 3 and the results of solder heat resistance measurement. In the table, the minimum melt viscosity of the polyester film on the surface is measured by an overhead flow tester. (The temperature increase rate is 2 ° C / min.) The maximum size of the resin concentration is the maximum size of the fixed part that is hardened at the observation length of the cross-section observation length of the test piece 10 cm. 0 The heat resistance of the solder According to JIS-C 5 0 1 3, the heat resistance of the test piece on molten solder (2 60 ° C) and the time until air bubbles appeared on the surface of the test piece (η = 5 average 値) was measured. It is not shown in Table 1. However, in each example, in the central layer, an average of 120 to 180 resin concentration points (fixed sections) were formed in 100 cm 2. The Intellectual Property Bureau, Ministry of Economic Affairs, Consumer Consumption Cooperatives Printing from Table 1 It is clearly understood that in each of the embodiments of the present invention, a good resin concentration (fixed portion) is formed, which has excellent solder heat resistance. Secondly, if you look at Examples 2 to 5, you can see that even if it contains more than 0.1 %, The second epoxy resin composition containing aluminum hydroxide of 0.1 to 16% by mass of impure sodium oxide can also provide good solder heat resistance. Also, aluminum hydroxide (containing less than 0.1% by mass of impure sodium oxide) Example 1 of the second epoxy resin composition on the polyester film of the center layer can be seen from comparison with Example 1 using conventional aluminum hydroxide having the same high heat resistance. The solder heat resistance in Example 1 can be improved more than in the previous Example 1. This paper applies the Chinese National Standard (CNS) A4 specification (210X297 mm) -13-567139 A7 B7 V. Description of the invention (j [Invention Effect] As described above, the synthetic laminate of the present invention is based on the epoxy resin composition in the center layer, and although it contains aluminum hydroxide as an inorganic filler, it is due to the epoxy resin in the surface layer. The composition extends to the central layer in a state of being connected to the surface layer, and constitutes a concentrated resin portion (fixed portion) distributed in the central layer, so the heat resistance is excellent. The method of the present invention is for manufacturing the aforementioned structure. Synthetic laminated board is an effective method. [Simplified description of the drawing] Fig. 1 is a cross-sectional explanatory view showing a synthetic laminated board according to an embodiment of the present invention in a pattern. [Illustration of drawing number] 1: Surface layer 2: Center Layer 3: Resin Concentration (Fixed Department) (Please read the notes on the back before filling out this page) Printed by the Employees' Cooperatives of the Intellectual Property Bureau of the Ministry of Economic Affairs This paper is printed in accordance with China National Standard (CNS) A4 (210X297 mm) • 14-