TWI602843B - A resin composition, a prepreg using the same, a laminate, and a printed wiring board - Google Patents
A resin composition, a prepreg using the same, a laminate, and a printed wiring board Download PDFInfo
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- TWI602843B TWI602843B TW105110764A TW105110764A TWI602843B TW I602843 B TWI602843 B TW I602843B TW 105110764 A TW105110764 A TW 105110764A TW 105110764 A TW105110764 A TW 105110764A TW I602843 B TWI602843 B TW I602843B
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- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K5/00—Use of organic ingredients
- C08K5/16—Nitrogen-containing compounds
- C08K5/34—Heterocyclic compounds having nitrogen in the ring
- C08K5/3412—Heterocyclic compounds having nitrogen in the ring having one nitrogen atom in the ring
- C08K5/3415—Five-membered rings
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- 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
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
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- 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
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- 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
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- 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
- B32B15/092—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 comprising epoxy resins
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- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/06—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material
- B32B27/08—Layered products comprising a layer of synthetic resin 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
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- 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
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/28—Layered products comprising a layer of synthetic resin comprising synthetic resins not wholly covered by any one of the sub-groups B32B27/30 - B32B27/42
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B33/00—Layered products characterised by particular properties or particular surface features, e.g. particular surface coatings; Layered products designed for particular purposes not covered by another single class
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- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
- C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
- C08G59/40—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the curing agents used
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- C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
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- C—CHEMISTRY; METALLURGY
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- C08J5/24—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs
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- C08K5/17—Amines; Quaternary ammonium compounds
- C08K5/18—Amines; Quaternary ammonium compounds with aromatically bound amino groups
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- C08L79/04—Polycondensates having nitrogen-containing heterocyclic rings in the main chain; Polyhydrazides; Polyamide acids or similar polyimide precursors
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- C08L83/04—Polysiloxanes
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- 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
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- 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
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- 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
- H05K1/0373—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement containing additives, e.g. fillers
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- B32B2255/00—Coating on the layer surface
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- B32B2307/30—Properties of the layers or laminate having particular thermal properties
- B32B2307/306—Resistant to heat
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- B32B2307/50—Properties of the layers or laminate having particular mechanical properties
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- B32B2457/00—Electrical equipment
- B32B2457/08—PCBs, i.e. printed circuit boards
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- C08J2479/04—Polycondensates having nitrogen-containing heterocyclic rings in the main chain; Polyhydrazides; Polyamide acids or similar polyimide precursors
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- Epoxy Resins (AREA)
- Macromolecular Compounds Obtained By Forming Nitrogen-Containing Linkages In General (AREA)
- Laminated Bodies (AREA)
Description
本發明係關於一種樹脂組成物,其係具有絕緣性或耐熱性等之同時特別是低熱膨脹性優異且是使用於電子零件等者;以及使用此樹脂組成物的預浸體、層合板、印刷配線板。
隨著近年的電子機器之小型化、高性能化之潮流,印刷配線板朝向配線密度之高度化、高積體化進展著,伴隨於此,對於藉由配線用層合板之耐熱性提昇之可靠性提昇,正強烈地被要求著。在如此般之用途中,要求著兼具優異的耐熱性、低線膨脹係數。
作為印刷配線板用層合板,一般係將以環氧樹脂作為基底樹脂的樹脂組成物及玻璃織布進行硬化、一體成形者。一般而言,環氧樹脂之絕緣性或耐熱性、成本等之平衡優異,但在對應於隨著近年印刷配線板之高密度安裝、高多層化構成而對於耐熱性提昇提出之要求上,其耐熱性之上昇終究是有限的。更,由於熱膨脹率大,故藉由具有芳香環之環氧樹脂之選擇或將矽石等
無機填充材進行高填充化來試圖低熱膨脹化(參考例如專利文獻1)。
特別是近年,在半導體用封裝基板,伴隨著小型化、薄型化,於零件安裝時或封裝組裝時,起因於晶片與基板之熱膨脹係數之差之翹曲,已成為大課題,正要求著低熱膨脹化,但增加無機填充材之填充量,已知有因吸濕而絕緣可靠性降低或樹脂-配線層之密著力不足、加壓成形不良之產生。
又,廣泛地使用於高密度安裝、高多層化層合板之聚雙馬來醯亞胺樹脂,雖然其耐熱性非常優異,但吸濕性高,黏著性上有缺點。更,於層合時,相較於環氧樹脂,需要更高溫、更長時間,而具有生產性差之缺點。
即,一般而言,環氧樹脂時,可在180℃以下之溫度進行硬化,但若為層合聚雙馬來醯亞胺樹脂時,需要220℃以上之高溫且長時間之處理。又,改質醯亞胺樹脂組成物,雖然是耐濕性或黏著性已改良(參考例如專利文獻2),但由於是為了確保對於甲基乙基酮等泛用性溶劑之可溶性而使用含有羥基及環氧基之低分子化合物來進行改質,故所得到的改質醯亞胺樹脂之耐熱性,相較於聚雙馬來醯亞胺樹脂大幅地變差。
[專利文獻1]日本特開平5-148343號公報
[專利文獻2]日本特開平6-263843號公報
有鑑於如此般之現狀,本發明之目的係以提供一特別是耐熱性、低熱膨脹性優異之樹脂組成物,以及使用此的預浸體、層合板、印刷配線板。
本發明人們為了達成前述目的,經不斷深入研究之結果,發現一種樹脂組成物,其係含有聚雙馬來醯亞胺樹脂及具有反應性有機基之聚矽氧樹脂,可達成上述目的。
即,本發明為提供以下的樹脂組成物、預浸體層合板及印刷配線板。
1.一種樹脂組成物,其特徵係含有(a)一分子構造中具有至少2個N-取代馬來醯亞胺基之馬來醯亞胺化合物、及(b)一分子構造中具有至少1個反應性有機基之聚矽氧化合物。
2.如上述1之樹脂組成物,其中,進而含有(c)熱硬化性樹脂。
3.如上述1或2之樹脂組成物,其中,進而含有(d)下述一般式(I)所示具有酸性取代基之胺化合物。
(式中,R1若為複數個時,分別獨立示為作為酸性取代基之羥基、羧基或磺酸基,R2若為複數個時,分別獨立示為氫原子、碳數1~5之脂肪族烴基或鹵素原子,x為1~5之整數、y為0~4之整數、x+y=5)。
4.如上述1~3項中任一項之樹脂組成物,其中,(b)成分為含有下述一般式(II)所示構造之聚矽氧化合物。
[式中,R3、R4分別獨立示為烷基、苯基或取代苯基,n為1~100之整數]。
5.如上述1~4項中任一項之樹脂組成物,其中,(b)成分之反應性有機基為選自環氧基、胺基、羥基、甲基丙烯酸基、巰基、羧基、烷氧基之至少一種。
6.如上述1~5項中任一項之樹脂組成物,其中,(b)成分為一分子構造中具有至少2個反應性有機基之聚矽氧化合物。
7.如上述1~5項中任一項之樹脂組成物,其中,(b)成分為兩末端具有反應性有機基之聚矽氧化合物。
8.如上述1~5項中任一項之樹脂組成物,其中,(b)成分為任一方之末端具有反應性有機基之聚矽氧化合物。
9.如上述1~5項中任一項之樹脂組成物,其中,(b)成分為側鏈具有反應性有機基之聚矽氧化合物。
10.如上述1~5項中任一項之樹脂組成物,其中,(b)成分為側鏈及至少一方之末端具有反應性有機基之聚矽氧化合物。
11.如上述1~10項中任一項之樹脂組成物,其中,(c)成分為分子構造中具有環氧基及/或氰酸酯基之熱硬化性樹脂。
12.如上述1~11項中任一項之樹脂組成物,其中,進而含有下述一般式(III)或(IV)所示(e)硬化促進劑。
(式中,R6、R7、R8、R9分別獨立示為氫原子、碳數1~5之脂肪族烴基或苯基,D為伸烷基或芳香族烴基)。
(式中,R6、R7、R8、R9分別獨立示為氫原子或碳數1~5之脂肪族烴基、苯基,B為單鍵或伸烷基、亞烷基、醚基、磺醯基中任一種)。
13.如上述1~12項中任一項之樹脂組成物,其中,進而含有(f)無機填充材。
14.一種預浸體,其係使用如上述1~13項中任一項之樹脂組成物。
15.一種層合板,其係使用如上述14之預浸體來進行層合成形而得到。
16.一種印刷配線板,其係使用如上述15之層合板而製造。
將本發明之樹脂組成物含浸或塗佈於基材而得到的預浸體,及藉由將該預浸體進行層合成形而製造的層合板,及使用該層合板而製造的多層印刷配線板,玻璃轉移溫度、熱膨脹率、焊料耐熱性、翹曲特性優異,且作為電子機器用印刷配線板為有用的。
以下,對於本發明進行詳細說明。本發明為一種樹脂組成物,其特徵係含有(a)一分子構造中具有至少2個N-取代馬來醯亞胺基之馬來醯亞胺化合物、及(b)一分子構造中具有至少1個反應性有機基之聚矽氧化合物。
作為本發明之樹脂組成物之(a)成分之一分子中具有至少2個N-取代馬來醯亞胺基之馬來醯亞胺化合物,例如可舉例N,N'-伸乙基雙馬來醯亞胺、N,N'-六亞甲基雙馬來醯亞胺、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-馬來醯亞胺苯基)甲烷、雙(3-甲基-4-馬來醯亞胺苯基)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-馬來醯亞胺苯基)醚、雙(4-馬來醯亞胺苯基)碸、雙(4-馬來醯亞胺苯基)硫醚、雙(4-馬來醯亞胺苯基)酮、雙(4-馬來醯亞胺環己基)甲烷、1,4-雙(4-馬來醯亞胺苯基)環己烷、1,4-雙(馬來醯亞胺甲基)環己烷、1,4-雙(馬來醯亞胺甲基)苯、1,3-雙(4-馬來醯亞胺苯氧基)苯、1,3-雙(3-馬來醯亞胺苯氧基)苯、雙[4-(3-馬來醯亞胺苯氧基)苯基]甲烷、雙[4-(4-馬來醯亞胺苯氧基)苯基]甲烷、1,1-雙[4-(3-馬來醯亞胺苯氧基)苯基]乙烷、1,1-雙[4-(4-馬來醯亞胺苯氧基)苯基]乙烷、1,2-雙[4-(3-馬來醯亞胺苯氧基)苯基]乙烷、1,2-雙[4-(4-馬來醯亞胺苯氧基)苯基]乙烷、2,2-雙[4-(3-馬來醯亞胺苯氧基)苯基]丙烷、2,2-雙[4-(4-馬來醯亞胺苯氧基)苯基]丙烷、2,2-雙[4-(3-馬來醯亞胺苯氧基)苯基]丁烷、2,2-雙[4-(4-馬來醯亞胺苯氧基)苯基]丁烷、2,2-雙[4-(3-馬來醯亞胺苯氧基)苯基]-1,1,1,3,3,3-六氟丙烷、2,2-雙[4-(4-馬來醯亞胺苯氧基)苯基]-1,1,1,3,3,3-六氟丙烷、4,4-雙(3-馬來醯亞胺苯氧基)聯苯、4,4-雙(4-馬來醯亞胺苯氧基)聯苯、雙[4-(3-馬來醯亞胺苯氧基)苯基]酮、雙[4-(4-馬來醯亞胺苯氧基)苯基]酮、2,2-雙(4-馬
來醯亞胺苯基)二硫醚、雙(4-馬來醯亞胺苯基)二硫醚、雙[4-(3-馬來醯亞胺苯氧基)苯基]硫醚、雙[4-(4-馬來醯亞胺苯氧基)苯基]硫醚、雙[4-(3-馬來醯亞胺苯氧基)苯基]亞碸、雙[4-(4-馬來醯亞胺苯氧基)苯基]亞碸、雙[4-(3-馬來醯亞胺苯氧基)苯基]碸、雙[4-(4-馬來醯亞胺苯氧基)苯基]碸、雙[4-(3-馬來醯亞胺苯氧基)苯基]醚、雙[4-(4-馬來醯亞胺苯氧基)苯基]醚、1,4-雙[4-(4-馬來醯亞胺苯氧基)-α,α-二甲基苄基]苯、1,3-雙[4-(4-馬來醯亞胺苯氧基)-α,α-二甲基苄基]苯、1,4-雙[4-(3-馬來醯亞胺苯氧基)-α,α-二甲基苄基]苯、1,3-雙[4-(3-馬來醯亞胺苯氧基)-α,α-二甲基苄基]苯、1,4-雙[4-(4-馬來醯亞胺苯氧基)-3,5-二甲基-α,α-二甲基苄基]苯、1,3-雙[4-(4-馬來醯亞胺苯氧基)-3,5-二甲基-α,α-二甲基苄基]苯、1,4-雙[4-(3-馬來醯亞胺苯氧基)-3,5-二甲基-α,α-二甲基苄基]苯、1,3-雙[4-(3-馬來醯亞胺苯氧基)-3,5-二甲基-α,α-二甲基苄基]苯、聚苯基甲烷馬來醯亞胺(例如,大和化成(股)製、商品名:BMI-2300等),此等馬來醯亞胺化合物可以單獨使用或混合2種類以上使用。
此等馬來醯亞胺化合物之中,以反應率高且可更高耐熱性化之雙(4-馬來醯亞胺苯基)甲烷、雙(4-馬來醯亞胺苯基)碸、N,N'-(1,3-伸苯基)雙馬來醯亞胺、2,2-雙(4-(4-馬來醯亞胺苯氧基)苯基)
丙烷、聚苯基甲烷馬來醯亞胺為佳;就對於溶劑之溶解性方面而言,特佳為雙(4-馬來醯亞胺苯基)甲烷。
作為(b)成分之一分子構造中具有至少1個反應性有機基之聚矽氧化合物,有含有下述一般式(II)所示構造之聚矽氧化合物。
[式中,R3、R4分別獨立示為烷基、苯基或取代苯基,n為1~100之整數]。
作為(b)成分,適合使用一分子構造中具有至少2個反應性有機基之聚矽氧化合物,可使用如上述般之聚矽氧構造之兩末端具有反應性有機基之聚矽氧化合物、任一方之末端具有反應性有機基之聚矽氧化合物或側鏈具有反應性有機基之聚矽氧化合物、側鏈及至少一方之末端具有反應性有機基之聚矽氧化合物。
作為(b)成分之一分子構造中具有至少1個反應性有機基之聚矽氧化合物之反應性有機基,舉例如環氧基、胺基、羥基、甲基丙烯酸基、巰基、羧基、烷氧基。
分子構造中具有環氧基之聚矽氧化合物,可使用市售品,例如可舉例兩末端具有環氧基之「X-22-163」(官能基當量200)、「KF-105」(官能基當量490)、「X-22-163A」(官能基當量1000)、「X-22-163B」(官能基當量1750)、「X-22-163C」(官能基當量2700);兩末端具有脂環式環氧基之「X-22-169AS」(官能基當量500)、「X-22-169B」(官能基當量1700);一方之末端具有環氧基之「X-22-1730X」(官能基當量4500);側鏈及兩末端具有環氧基之「X-22-9002」(官能基當量5000);側鏈具有環氧基之「X-22-343」(官能基當量525)、「KF-101」(官能基當量350)、「KF-1001」(官能基當量3500)、「X-22-2000」(官能基當量620)、「X-22-4741」(官能基當量2500)、「KF-1002」(官能基當量4300);側鏈具有脂環式環氧基之「X-22-2046」(官能基當量600)、「KF-102」(官能基當量3600、以上為信越化學工業(股)製),此等可以單獨使用、混合2種類以上使用、進而與各種環氧樹脂混合來使用。
此等分子構造中具有環氧基之聚矽氧化合物之中,就耐熱性方面而言,較佳為「X-22-163A」、「X-22-163B」、「X-22-343」、「X-22-9002」、「KF-101」,更佳為「X-22-163A」、「X-22-
163B」;就低熱膨脹率方面而言,特佳為「X-22-163B」。
分子構造中具有胺基之聚矽氧化合物,可使用市售品,例如可舉例兩末端具有胺基之「KF-8010」(官能基當量430)、「X-22-161A」(官能基當量800)、「X-22-161B」(官能基當量1500)、「KF-8012」(官能基當量2200)、「KF-8008」(官能基當量5700)、「X-22-9409」(官能基當量700)、「X-22-1660B-3」(官能基當量2200)(以上為信越化學工業(股)製)、「BY-16-853U」(官能基當量460)、「BY-16-853」(官能基當量650)、「BY-16-853B」(官能基當量2200)(以上為Dow Corning Toray(股)製);側鏈具有胺基之「KF-868」(官能基當量8800)、「KF-865」(官能基當量5000)、「KF-864」(官能基當量3800)、「KF-880」(官能基當量1800)、「KF-8004」(官能基當量1500)(以上為信越化學工業(股)製),此等可以單獨或混合2種類以上使用。
此等分子構造中具有胺基之聚矽氧化合物之中,就低吸水率方面而言,較佳為X-22-161A、X-22-161B、KF-8012、KF-8008、X-22-1660B-3、BY-16-853B;就低熱膨脹性方面而言,特佳為X-22-161A、X-22-161B、KF-8012。
分子構造中具有羥基之聚矽氧化合物,可使用市售品,例如可舉例兩末端具有羥基之「KF-6001」(官能基當量900)、「KF-6002」(官能基當量1600);兩末端具有酚性羥基之「X-22-1821」(官能基當量1470)(以上為信越化學工業(股)製)、「BY-16-752A」(官能基當量1500)(以上為Dow Corning Toray(股)製);一方之末端具有羥基之「X-22-170BX」(官能基當量2800)、「X-22-170DX」(官能基當量4670);側鏈具有羥基之「X-22-4039」(官能基當量970)「X-22-4015」(官能基當量1870)(以上為信越化學工業(股)製),此等可以單獨或混合2種類以上使用。
分子構造中具有甲基丙烯酸基之聚矽氧化合物,可使用市售品,例如可舉例兩末端具有甲基丙烯酸基之「X-22-164A」(官能基當量860)、「X-22-164B」(官能基當量1630);一方之末端具有甲基丙烯酸基之「X-22-174DX」(官能基當量4600)(以上為信越化學工業(股)製),此等可以單獨或混合2種類以上使用。
分子構造中具有巰基之聚矽氧化合物,可使用市售品,例如可舉例兩末端具有巰基之「X-22-167B」(官能基當量1670);側鏈具有巰基之「KF-2001」(官能基當量1900)、「KF-2004」(官能
基當量30000)(以上為信越化學工業(股)製),此等可以單獨或混合2種類以上使用。
分子構造中具有羧基之聚矽氧化合物,可使用市售品,例如可舉例兩末端具有羧基之「X-22-162C」(官能基當量2300);一方之末端具有羧基之「X-22-3710」(官能基當量1450);側鏈具有羧基之「X-22-3701E」(官能基當量4000)(以上為信越化學工業(股)製),此等可以單獨或混合2種類以上使用。
分子構造中具有烷氧基之聚矽氧化合物,可使用市售品,例如可舉例側鏈具有烷氧基之「FZ-3704」(官能基當量150)(以上為Dow Corning Toray(股)製),此等可以單獨或混合2種類以上使用。
(b)成分之使用量,相對於(a)成分100質量份,較佳為1~100質量份、更佳為5~80質量份。藉由設定為1質量份以上,可使低熱膨脹率化成為可能。藉由設定為100質量份以下,可確保銅箔密著性或成形性。
本發明之樹脂組成物中,較佳為進而含有(c)熱硬化性樹脂。(c)成分之熱硬化性樹脂,未特別限制,例如可舉例環氧樹脂、酚樹脂、不飽和醯亞胺樹脂、氰酸酯樹脂、異氰酸酯樹脂、苯并噁嗪(benzoxazine)樹脂、氧雜環丁烷樹脂、胺基樹脂、不
飽和聚酯樹脂、烯丙基樹脂、二環戊二烯樹脂、聚矽氧樹脂、三嗪(triazine)樹脂、三聚氰胺樹脂,此等可以單獨或混合2種類以上使用。此等之中,就成形性或電氣絕緣性方面而言,較佳為環氧樹脂、氰酸酯樹脂。
作為環氧樹脂,例如可舉例雙酚A型環氧樹脂、雙酚F型環氧樹脂、雙酚S型環氧樹脂、苯酚酚醛型環氧樹脂、甲酚酚醛型環氧樹脂、雙酚A酚醛型環氧樹脂、雙酚F酚醛型環氧樹脂、二苯乙烯型環氧樹脂、含三嗪骨架之環氧樹脂、含芴骨架之環氧樹脂、三酚酚甲烷型環氧樹脂、聯苯型環氧樹脂、伸茬基型環氧樹脂、聯苯芳烷基型環氧樹脂、萘型環氧樹脂、二環戊二烯型環氧樹脂、脂環式環氧樹脂、多官能酚類及蒽等多環芳香族類之二縮水甘油醚化合物,及將磷化合物導入於此等中而成之含磷環氧樹脂,此等可以單獨或混合2種類以上使用。此等之中,就耐熱性、難燃性方面而言,較佳為聯苯芳烷基型環氧樹脂、萘型環氧樹脂。
又,作為氰酸酯樹脂,例如可舉例酚醛型氰酸酯樹脂、雙酚A型氰酸酯樹脂、雙酚E型氰酸酯樹脂、四甲基雙酚F型氰酸酯樹脂等雙酚型氰酸酯樹脂及此等之一部分經三嗪化之預聚物,此等可以單獨或混合2種類以上使用。此等之中,就耐熱性、難燃性方面而言,較佳為酚醛型氰酸酯樹脂。
(c)成分之使用量,相對於(a)成分100質量份,較佳為10~200質量份、更佳為20~100質
量份。藉由設定為10質量份以上,可得到優異的吸濕特性或銅箔密著性。藉由設定為200質量份以下,可確保耐熱性,並使低熱膨脹率化成為可能的。
本發明之樹脂組成物中,較佳為進而含有作為(d)成分之下述一般式(I)所示具有酸性取代基之胺化合物。
(式中,R1若為複數個時,分別獨立示為作為酸性取代基之羥基、羧基或磺酸基,R2若為複數個時,分別獨立示為氫原子、碳數1~5之脂肪族烴基或鹵素原子,x為1~5之整數、y為0~4之整數、x+y=5)。
作為(d)成分之胺化合物,例如可舉例m-胺基苯酚、p-胺基苯酚、o-胺基苯酚、p-胺基安息香酸、m-胺基安息香酸、o-胺基安息香酸、o-胺基苯磺酸、m-胺基苯磺酸、p-胺基苯磺酸、3,5-二羥基苯胺、3,5-二羧基苯胺,此等之中,就溶解性或合成之收率方面而言,較佳為m-胺基苯酚、p-胺基苯酚、o-胺基苯酚、p-胺基安息香酸、m-胺基安息香酸及3,5-二
羥基苯胺,就耐熱性方面而言,更佳為m-胺基苯酚及p-胺基苯酚。
(d)成分之使用量,相對於(a)成分100質量份,較佳為0.1~20質量份、更佳為1~10質量份。藉由設定為0.1質量份以上,可得到優異的耐熱性或銅箔密著性。藉由設定為20質量份以下,可確保耐熱性。
(d)成分,較佳為事先與(a)成分進行反應。此反應中所使用的有機溶劑,未特別限制,例如可舉例乙醇、丙醇、丁醇、甲基賽路蘇、丁基賽路蘇、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;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;甲基甲醯胺、二甲基乙醯胺、N-甲基吡咯啶酮等含氮原子之溶劑;二甲基亞碸等含硫原子之溶劑,此等可以單獨或混合2種類以上使用。此等之中,就溶解性方面而言,較佳為環己酮、丙二醇單甲基醚、甲基賽路蘇,就低毒性之方面而言,更佳為環己酮、丙二醇單甲基醚,就揮發性高,且於預浸體之製造時不易殘留作為殘留溶劑,特佳為丙二醇單甲基醚。
又,前述反應中,可依據需要而任意使用反應觸媒,未特別限定。作為反應觸媒之例,舉例如三乙基胺、吡啶、三丁基胺等胺類;甲基咪唑、苯基咪唑等
咪唑類;三苯基膦等磷系觸媒,此等可以單獨或混合2種類以上使用。
使(a)成分及(d)成分於有機溶劑中進行反應之際,反應溫度較佳為70~150℃、更佳為100~130℃。反應時間,較佳為0.1~10小時、更佳為1~6小時。
本發明之樹脂組成物中,為了提昇耐熱性或難燃性、銅箔黏著性等,宜為使用(e)硬化促進劑,作為硬化促進劑之例,舉例如咪唑類及其衍生物、第三級胺類及第四級銨鹽等。
之中又以咪唑類及其衍生物,就耐熱性或難燃性、銅箔黏著性等之方面來說較佳;而且下述一般式(III)所示異氰酸酯樹脂,或下述一般式(IV)所示咪唑基經環氧樹脂所取代之化合物,由於在200℃以下之較為低溫之硬化成形性及清漆或預浸體之經日安定性優異,故更佳;具體可少量摻合下述式(V)或式(VI)所示化合物來使用,又,由於商業上亦為廉價,故特佳。
(式中,R6、R7、R8、R9分別獨立示為氫原子、碳數1~5之脂肪族烴基或苯基,D為伸烷基或芳香族烴基)。
(式中,R6、R7、R8、R9分別獨立示為氫原子或碳數1~5之脂肪族烴基、苯基,B為單鍵或伸烷基、亞烷基、醚基、磺醯基中任一種)。
(e)硬化促進劑之使用量,相對於固形物換算之(a)~(d)成分之總和每100質量份,較佳設定為0.1~10質量份、更佳設定為0.1~5質量份、特佳設定為0.1~1質量份。藉由將硬化促進劑之使用量設定為0.1質量份以上,可得到優異的耐熱性或難燃性、銅箔黏著性,又,藉由設定為10質量份以下,耐熱性、經日安定性及加壓成形性不會降低。
本發明之樹脂組成物中,可任意併用(f)無機填充材。作為無機填充材,舉例如矽石、氧化鋁、滑石、雲母、高嶺土、氫氧化鋁、水鋁礦、氫氧化鎂、硼酸鋅、錫酸鋅、氧化鋅、氧化鈦、氮化硼、碳酸鈣、硫酸鋇、硼酸鋁、鈦酸鉀、E玻璃或T玻璃、D玻璃等之玻璃粉或中空玻璃珠粒等,此等可以單獨或混合2種類以上使用。
在此等(f)成分之無機填充材中,就介電特性、耐熱性、低熱膨脹性方面而言,特佳為矽石。作為矽石,可舉例使用濕式法所製造含水率為高的沈降矽石及使用乾式法所製造幾乎不含結合水等的乾式法矽石;作為乾式法矽石,依製造法之不同,進而可舉例破碎矽石、燻製矽石、熔融球狀矽石。此等之中,就低熱膨脹性及填充於樹脂之際之高流動性而言,較佳為熔融球狀矽石。
若使用熔融球狀矽石作為無機填充材時,其平均粒徑較佳為0.1~10μm、更佳為0.3~8μm。藉
由將該熔融球狀矽石之平均粒徑設定為0.1μm以上,可確保於樹脂中進行高填充時之良好流動性,而且藉由設定為10μm以下,可降低粗大粒子之混入機率並抑制起因於粗大粒子之不良之發生。在此,所謂的平均粒徑,係將粒子之全體積作為100%,並依粒徑求得累積次數分佈曲線時,正好為相當於體積50%之點之粒徑者,可藉由使用雷射繞射散射法之粒度分佈測定裝置等來進行測定。
(f)無機填充材之含有量,相對於固形物換算之(a)~(d)成分之總和每100質量份,較佳為10~300質量份、更佳為50~250質量份。藉由將無機填充材之含有量設定為相對於樹脂成分之總和每100質量份為10~300質量份,可確保樹脂組成物之良好成形性及低熱膨脹性。
本發明在不違背其目的之範圍內,可併用任意周知的熱可塑性樹脂、彈性物、難燃劑、有機填充材等。
作為熱可塑性樹脂之例,舉例如聚四氟乙烯、聚乙烯、聚丙烯、聚苯乙烯、聚苯醚(polyphenyleneether)樹脂、苯氧樹脂、聚碳酸酯樹脂、聚酯樹脂、聚醯胺樹脂、聚醯亞胺樹脂、二甲苯樹脂、石油樹脂及聚矽氧樹脂。
作為彈性物之例,舉例如聚丁二烯、聚丙烯腈、環氧改質聚丁二烯、順丁烯二酸酐改質聚丁二烯、酚改質聚丁二烯及羧基改質聚丙烯腈等。
作為有機填充材之例,舉例如聚矽氧粉末、四氟乙烯、聚乙烯、聚丙烯、聚苯乙烯以及聚苯醚等之有機物粉末等。
在本發明中,亦可任意地添加紫外線吸收劑、抗氧化劑、光聚合起始劑、螢光增白劑及密著性提昇劑等,未特別限定。作為此等之例,舉例如苯并三唑系等之紫外線吸收劑;受阻酚系或苯乙烯化酚等之抗氧化劑;二苯基酮類、苄基縮酮類、噻吨酮(thioxanthone)系等之光聚合起始劑;二苯乙烯衍生物等之螢光增白劑;尿素矽烷等之尿素化合物或矽烷偶合劑之密著性提昇劑。
本發明之樹脂組成物,於製造預浸體之際,係作為清漆來使用。對於清漆中所使用之溶劑,為使用與前述反應中所使用者為相同之溶劑。清漆在固形物濃度方面,較佳為以50~75質量%來進行使用。
本發明之預浸體,係將前述本發明之樹脂組成物含浸或塗佈於基材所成者。以下,對於本發明之預浸體進行詳述。
本發明之預浸體,可將本發明之樹脂組成物含浸或塗佈於基材,並藉由加熱等進行半硬化(B階段化)而製造。作為在此所使用的基材,可使用於各種電氣絕緣
材料用層合板中所使用的周知者。作為其材質之例,舉例如E玻璃、D玻璃、S玻璃及Q玻璃等之無機物纖維;聚醯亞胺、聚酯及聚四氟乙烯等之有機纖維;及此等之混合物。
此等基材,例如具有織布、不織布、粗紗、切股氈及表面氈等之形狀,材質及形狀為依照作為目的之成形物之用途或性能而選擇,依據需要,可以單獨或組合2種類以上之材質及形狀。基材之厚度未特別限制,例如,可使用約0.03~0.5mm,經以矽烷偶合劑等進行表面處理者或施以機械性開纖處理者,就耐熱性或耐濕性、加工性方面而言,為較佳。
本發明之預浸體,可以對於該基材之樹脂組成物之附著量以乾燥後之預浸體之樹脂含有率成為20~90質量%般地,含浸或塗佈於基材後,通常,以100~200℃之溫度加熱乾燥1~30分鐘使半硬化(B階段化)而得到。
本發明之層合板,可使用前述本發明之預浸體來進行層合成形而形成。可藉由將本發明之預浸體例如以重疊1~20張並於其單面或雙面配置銅及鋁等金屬箔之構成進行層合成形而製造。金屬箔,只要是在電氣絕緣材料用途所使用者即可,未特別限制。
製造層合板之際之成形條件,例如可將電氣絕緣材料用層合板及多層板之手法予以適用,例如可使用多段加壓、多段真空加壓、連續成形機、高壓釜成形機,並
以溫度100~250℃、壓力0.2~10MPa、加熱時間0.1~5小時之範圍,而進行成形。又,亦可組合本發明之預浸體及內層用配線板來進行層合成形,而製造層合板。
本發明相關之印刷配線板,係於前述層合板之表面形成電路而製造。即,將本發明相關之層合板之導體層,藉由通常的蝕刻法來進行配線加工,並隔著前述預浸體,將已配線加工之層合板予以複數層合,並藉由加熱加壓加工而一併進行多層化。之後,可經過藉由鑽孔加工或雷射加工而形成貫穿孔或盲通孔、及藉由鍍覆或導電性糊料而形成層間配線,製造多層印刷配線板。
接著,藉由下述的實施例將本發明更詳細地進行說明,惟,本發明並不限制於此等實施例。
尚,使用以各實施例及比較例所得到的貼銅層合板,對於玻璃轉移溫度、熱膨脹率、焊料耐熱性、翹曲特性,係使用以下之方法來測定、評估。
藉由將貼銅層合板浸漬於銅蝕刻液中,以製作已除去銅箔的5mm見方的評估基板,並使用TMA試驗裝置(Dupont公司製、TMA2940)藉由壓縮法來進行熱機械分析。將評估基板安裝於前述裝置之Z方向後,以荷重5g、昇溫速度10℃/分鐘之測定條件連續進行2
次測定。求得在第2次測定之熱膨脹曲線之相異切線之交點所示的Tg,來評估耐熱性。
藉由將貼銅層合板浸漬於銅蝕刻液中,以製作已除去銅箔的5mm見方的評估基板,並使用TMA試驗裝置(Dupont公司製、TMA2940)藉由壓縮法來進行熱機械分析。將評估基板安裝於前述裝置之X方向後,以荷重5g、昇溫速度10℃/分鐘之測定條件連續進行2次測定。算出第2次測定之由30℃至100℃的平均熱膨脹率,並將此作為熱膨脹率之值。
製作5cm見方的貼銅層合板,並將評估基板漂浮於溫度288℃之焊料浴中1分鐘後,藉由進行外觀觀察來評估焊料耐熱性。
使用AKROMETRIX公司製TherMoiré PS200 shadow moiré分析,來評估基板之翹曲量。將基板之樣品尺寸設定為40mm×40mm,測定區域設定為36mm×36mm。測定由室溫加熱至260℃之後冷卻至50℃時之翹曲量。
使用以下所示(a)~(d)成分與(e)硬化促進劑、(f)無機填充材及作為稀釋溶劑之甲基乙基酮,以
第1表~第5表所示的摻合比例(質量份)進行混合,而得到樹脂份65質量%之均勻清漆。
接著,將上述清漆含浸塗佈於厚度0.1mm之E玻璃布,並以160℃加熱乾燥10分鐘,而得到樹脂含有量50質量%之預浸體。
將此預浸體以4張重疊,並於上下配置18μm之電解銅箔,以壓力2.5MPa、溫度230℃進行90分鐘之加壓,而得到貼銅層合板。
所得到的貼銅層合板之測定、評估結果如第1表~第5表所示。
雙(4-馬來醯亞胺苯基)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
X-22-161A(信越化學工業(股)製、兩末端胺基改質、官能基當量800)
X-22-161B(信越化學工業(股)製、兩末端胺基改質、官能基當量1500)
KF-8012(信越化學工業(股)製、兩末端胺基改質、官能基當量2200)
KF-864(信越化學工業(股)製、單末端胺基改質、官能基當量3800)
X-22-163B(信越化學工業(股)製、兩末端環氧改質、官能基當量1750)
KF-6002(信越化學工業(股)製、兩末端羥基改質、官能基當量1600)
X-22-1821(信越化學工業(股)製、兩末端酚性羥基改質、官能基當量(1470)
X-22-164A(信越化學工業(股)製、兩末端甲基丙烯酸基改質、官能基當量860)
X-22-167B(信越化學工業(股)製、兩末端巰基改質、官能基當量1670)
X-22-162C(信越化學工業(股)製、兩末端羧基改質、官能基當量2300)
FZ-3704(Dow Corning Toray(股)製、側鏈烷氧基改質、官能基當量150)
聯苯芳烷基型環氧樹脂(日本化藥(股)製NC-3000)
雙酚A型氰酸酯樹脂(LONZA Japan(股)製B10)
m-胺基苯酚
p-胺基苯酚
G-8,009L(六亞甲基二異氰酸酯樹脂與2-乙基-4-甲基咪唑之加成反應物:以前述式(V)所示化合物)
二胺基二苯基甲烷(比較例)
2,2-雙[4-(胺基苯氧基)苯基]丙烷
由第1表~第5表可明確得知,本發明之實施例時,玻璃轉移溫度、熱膨脹率、焊料耐熱性、翹曲特性優異。另一方面,相較於實施例,比較例在玻璃轉移溫度、熱膨脹率、焊料耐熱性、翹曲特性中,任一種特性較差。
將由本發明之熱硬化性樹脂組成物所得到的預浸體進行層合成形而製造層合板,並使用該層合板而製造多層印刷配線板,該多層印刷配線板之玻璃轉移溫度、熱膨脹率、焊料耐熱性、翹曲特性優異,作為高積體化之電子機器用印刷配線板為有用的。
Claims (13)
- 一種預浸體,其係使用樹脂組成物而得到,該樹脂組成物含有(a)一分子構造中具有至少2個N-取代馬來醯亞胺基之馬來醯亞胺化合物、及(b)一分子構造中具有至少1個反應性的有機基之聚矽氧化合物,且,前述(b)成分為含有下述一般式(II)所示構造之聚矽氧化合物,
- 如請求項1之預浸體,其中,前述樹脂組成物含有(c)熱硬化性樹脂。
- 如請求項2之預浸體,其中,前述(c)成分為分子構造中具有環氧基及/或氰酸酯基之熱硬化性樹脂。
- 如請求項1~3中任一項之預浸體,其中,前述(b)成分之反應性的有機基為選自環氧基、胺基、羥基、甲基丙烯酸基、巰基、羧基、烷氧基之至少一種。
- 如請求項1~3中任一項之預浸體,其中,前述(b)成分為一分子構造中具有至少2個反應性的有機基之聚矽氧化合物。
- 如請求項1~3中任一項之預浸體,其中,前述(b)成分為兩末端具有反應性的有機基之聚矽氧化合物。
- 如請求項1~3中任一項之預浸體,其中,前述(b)成分為任一方之末端具有反應性的有機基之聚矽氧化合物。
- 如請求項1~3中任一項之預浸體,其中,前述(b)成分為側鏈具有反應性的有機基之聚矽氧化合物。
- 如請求項1~3中任一項之預浸體,其中,前述(b)成分為側鏈及至少一方之末端具有反應性的有機基之聚矽氧化合物。
- 如請求項1~3中任一項之預浸體,其中,前述樹脂組成物含有下述一般式(III)或(IV)所示(e)硬化促進劑,
- 如請求項1~3中任一項之預浸體,其中,前述樹脂組成物含有(f)無機填充材。
- 一種層合板,其係使用如請求項1~11中任一項之預浸體來進行層合成形而得到。
- 一種印刷配線板,其係使用如請求項12之層合板而製造。
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CN105647118B (zh) | 2020-06-26 |
JP6969843B2 (ja) | 2021-11-24 |
CN105504809A (zh) | 2016-04-20 |
TWI576365B (zh) | 2017-04-01 |
KR102127581B1 (ko) | 2020-06-26 |
CN105647118A (zh) | 2016-06-08 |
KR101832869B1 (ko) | 2018-04-13 |
JP6333791B2 (ja) | 2018-05-30 |
CN105602197A (zh) | 2016-05-25 |
JP2016028164A (ja) | 2016-02-25 |
TW201249885A (en) | 2012-12-16 |
WO2012099132A1 (ja) | 2012-07-26 |
TW201605921A (zh) | 2016-02-16 |
JP5831462B2 (ja) | 2015-12-09 |
JP2018028105A (ja) | 2018-02-22 |
CN103328577A (zh) | 2013-09-25 |
TWI541263B (zh) | 2016-07-11 |
KR20180023022A (ko) | 2018-03-06 |
KR20140006826A (ko) | 2014-01-16 |
TW201629118A (zh) | 2016-08-16 |
EP2666825A1 (en) | 2013-11-27 |
CN105602197B (zh) | 2020-11-20 |
JP6241536B2 (ja) | 2017-12-06 |
JP6270797B2 (ja) | 2018-01-31 |
JPWO2012099132A1 (ja) | 2014-06-30 |
CN105462253A (zh) | 2016-04-06 |
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