TWI698466B - 樹脂組成物、預浸體、樹脂片、覆金屬箔疊層板及印刷電路板 - Google Patents
樹脂組成物、預浸體、樹脂片、覆金屬箔疊層板及印刷電路板 Download PDFInfo
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- TWI698466B TWI698466B TW105121325A TW105121325A TWI698466B TW I698466 B TWI698466 B TW I698466B TW 105121325 A TW105121325 A TW 105121325A TW 105121325 A TW105121325 A TW 105121325A TW I698466 B TWI698466 B TW I698466B
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- 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
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- C08J7/043—Improving the adhesiveness of the coatings per se, e.g. forming primers
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Abstract
本發明提供一種成為耐化學性、耐除膠渣(desmear)性及絕緣可靠性優異之印刷電路板之原料的樹脂組成物。本發明之樹脂組成物包括馬來醯亞胺化合物、具有苯乙烯骨架與水解性基或苯乙烯骨架與羥基之矽烷化合物、以及無機填充材。
Description
本發明關於樹脂組成物、預浸體、樹脂片、覆金屬箔疊層板及印刷電路板。
近年,隨著廣泛使用於電子設備或通信器材、個人電腦等之半導體封裝的高機能化、小型化的發展,半導體封裝用之各零件的高積體化、高密度安裝化亦正日益加速中。與此同時,由於半導體元件與半導體塑膠封裝用印刷電路板間的熱膨脹率之差所產生的半導體塑膠封裝之翹曲成為問題,對此已尋求了各種對策。
其對策之一可列舉印刷電路板所使用之絕緣層的低熱膨脹化。其係藉由使印刷電路板之熱膨脹率接近於半導體元件之熱膨脹率以抑制翹曲的方法,現在正積極研究中(例如,參照專利文獻1~3)。
就抑制半導體塑膠封裝之翹曲的方法而言,除印刷電路板的低熱膨脹化以外,也有人研究將疊層板的剛性提高(高剛性化)、將疊層板的玻璃轉移溫度提高(高Tg化)(例如,參照專利文獻4及5)。 [先前技術文獻] [專利文獻]
專利文獻1:日本特開2013-216884號公報 專利文獻2:日本專利第3173332號公報 專利文獻3:日本特開2009-035728號公報 專利文獻4:日本特開2013-001807號公報 專利文獻5:日本特開2011-178992號公報
[發明所欲解決之課題] 但,伴隨半導體封裝用之各零件的高積體化、高密度安裝化所產生的課題不止上述,也有其他需研究的課題。例如,就自以往之技術而言,使預浸體與銅箔等金屬層疊層時,由於在蝕刻步驟、除膠渣步驟、鍍敷步驟等中疊層板暴露於藥液,若疊層板之耐化學性低的話,會有製品的品質、生產性差的問題。特別是在除膠渣步驟中,為了去除機械鑽孔加工、雷射鑽孔加工所產生的膠渣,係利用強鹼性的洗淨液。因此,若疊層板之耐化學性不充分的話,膠渣以外的通孔(through hole)內壁、其他樹脂層之表面也會溶出。其結果為以下的問題變得顯著:孔徑等所期望的加工變困難,或步驟受到污染而藥液的壽命變短,或絕緣層表面所形成之錨點(anchor)破壞而導致與導體層的黏合性降低(耐除膠渣性)。進一步,上述利用高Tg化的方法,伴隨因交聯密度上升所致之吸濕耐熱性的惡化,在要求非常高絕緣可靠性的電子材料領域中多有實用上的問題。又,就高Tg化的方法而言,宜採用提高馬來醯亞胺化合物之比率的方法,但此種情況下,變得難以抑制源自於馬來醯亞胺基之水解性的耐化學性的惡化。於是,在印刷電路板的製作中,要求具有優異的耐化學性、耐除膠渣性及絕緣可靠性。
本發明係鑒於上述情況而進行,旨在提供耐化學性、耐除膠渣性及絕緣可靠性優異的覆金屬箔疊層板及印刷電路板、以及成為該等之原材料的樹脂組成物、預浸體及樹脂片。 [解決課題之手段]
本案發明人們為了達成上述目的而進行努力研究的結果,發現藉由成為印刷電路板之原材料的樹脂組成物含有多個特定成分,可實現優異的耐化學性、耐除膠渣性及絕緣可靠性之全部,而完成了本發明。
亦即,本發明如下。 [1]一種樹脂組成物,包括馬來醯亞胺化合物、具有苯乙烯骨架與水解性基或苯乙烯骨架與羥基之矽烷化合物、以及無機填充材。 [2]如[1]之樹脂組成物,其中,包括下式(A)表示之化合物作為該矽烷化合物。 [化1](式中,R8
表示水解性基或羥基,R9
表示氫原子或碳數1~3之烷基,R8
或R9
有多數個時,多數個R8
或R9
彼此可相同也可不同,k表示1~3之整數。) [3]如[1]或[2]之樹脂組成物,更含有經烯基取代之納迪克醯亞胺。 [4]如[3]之樹脂組成物,其中,含有下式(1)表示之化合物作為該經烯基取代之納迪克醯亞胺。 [化2](式中,R1
各自獨立地表示氫原子、或碳數1~6之烷基,R2
表示碳數1~6之伸烷基、伸苯基、伸聯苯基、伸萘基、或下式(2)或(3)表示之基。) [化3](式中,R3
表示亞甲基、異亞丙基、CO、O、S、或SO2
表示之取代基。) [化4](式中,R4
各自獨立地表示碳數1~4之伸烷基、或碳數5~8之環伸烷基。) [5]如[3]或[4]之樹脂組成物,其中,包括下式(4)及/或(5)表示之化合物作為該經烯基取代之納迪克醯亞胺。 [化5][化6][6]如[1]~[5]中任一項之樹脂組成物,其中,包括選自於由雙(4-馬來醯亞胺苯基)甲烷、2,2-雙{4-(4-馬來醯亞胺苯氧基)-苯基}丙烷、雙(3-乙基-5-甲基-4-馬來醯亞胺苯基)甲烷及下式(6)表示之馬來醯亞胺化合物構成之群組中之至少1種化合物作為該馬來醯亞胺化合物。 [化7](式中,R5
各自獨立地表示氫原子或甲基,n1
表示1以上之整數。) [7]如[1]~[6]中任一項之樹脂組成物,更包括氰酸酯化合物。 [8]如[7]之樹脂組成物,其中,包括下式(7)及/或(8)表示之化合物作為該氰酸酯化合物。 [化8](式中,R6
各自獨立地表示氫原子或甲基,n2
表示1以上之整數。) [化9](式中,R7
各自獨立地表示氫原子或甲基,n3
表示1以上之整數。) [9]如[1]~[8]中任一項之樹脂組成物,其中,該無機填充材係預先利用該矽烷化合物進行了表面處理。 [10]如[1]~[9]中任一項之樹脂組成物,其中,該矽烷化合物之含量相對於該樹脂組成物中之構成樹脂之成分之合計100質量份為0.1~15質量份。 [11]如[1]~[10]中任一項之樹脂組成物,其中,該無機填充材包括選自於由二氧化矽、氧化鋁及氮化鋁構成之群組中之至少1種。 [12]如[1]~[11]中任一項之樹脂組成物,其中,該無機填充材之含量相對於該樹脂組成物中之構成樹脂之成分之合計100質量份為100~1100質量份。 [13]一種預浸體,具備:基材,及含浸或塗佈於該基材之如[1]~[12]中任一項之樹脂組成物。 [14]如[13]之預浸體,其中,該基材係選自於由E玻璃布、T玻璃布、S玻璃布、Q玻璃布及有機纖維布構成之群組中之至少1種。 [15]一種樹脂片,具備:支持體,及塗佈於該支持體之如[1]~[12]中任一項之樹脂組成物。 [16]一種疊層板,係重疊1片以上選自於由如[13]及[14]之預浸體、及如[15]之樹脂片構成之群組中之至少1種而得,包括選自於由該預浸體及該樹脂片構成之群組中之至少1種中所含之樹脂組成物之硬化物。 [17]一種覆金屬箔疊層板,具有:選自於由如[13]及[14]之預浸體、及如[15]之樹脂片構成之群組中之至少1種,以及配置在選自於由該預浸體及該樹脂片構成之群組中之至少1種之單面或兩面的金屬箔;包括選自於由該預浸體及該樹脂片構成之群組中之至少1種中所含之樹脂組成物之硬化物。 [18]一種印刷電路板,包括絕緣層及形成在該絕緣層之表面之導體層,該絕緣層包括如[1]~[12]中任一項之樹脂組成物。 [發明之效果]
根據本發明,可提供耐化學性、耐除膠渣性及絕緣可靠性優異的覆金屬箔疊層板及印刷電路板、以及成為該等之原材料的樹脂組成物、預浸體及樹脂片。
以下,針對實施本發明之形態(以下,簡稱為「本實施形態」。)進行詳細說明,但本發明並不限定於下列本實施形態。本發明在不脫離其要旨的範圍內可進行各種變形。
本實施形態之樹脂組成物包括馬來醯亞胺化合物、具有苯乙烯骨架與水解性基或苯乙烯骨架與羥基之矽烷化合物(以下,亦稱為「苯乙烯基系矽烷化合物」。)、以及無機填充材。該樹脂組成物,藉由包含馬來醯亞胺化合物與苯乙烯基系矽烷化合物,在水解性基或羥基部分鍵結於無機填充材的苯乙烯基系矽烷化合物進一步在苯乙烯骨架部分和馬來醯亞胺化合物鍵結,無機填充材與馬來醯亞胺化合物之間的黏合性高。特別是苯乙烯基系矽烷化合物與馬來醯亞胺化合物間的鍵結,據認為係起因於Diels-Alder加成所致之反應,藉此形成梯子形狀的交聯點,故據推測為更加牢固的鍵結。其結果為:對於本實施形態之樹脂組成物之藥品處理或除膠渣處理的耐性提升,可獲得耐化學性及耐除膠渣性優異的覆金屬箔疊層板及印刷電路板。進一步,除由於無機填充材與馬來醯亞胺化合物之間的高黏合性外,也由於苯乙烯基系矽烷化合物通常不具極性基而疏水性高,將本實施形態之樹脂組成物作為原材料而獲得之覆金屬箔疊層板及印刷電路板具有優異的絕緣可靠性。但,考慮的要因並不限定於上述。
本實施形態所使用之馬來醯亞胺化合物只要是於分子中具有1個以上之馬來醯亞胺基的化合物即可,並無特別限定。其具體例可列舉N-苯基馬來醯亞胺、N-羥基苯基馬來醯亞胺、雙(4-馬來醯亞胺苯基)甲烷、2,2-雙{4-(4-馬來醯亞胺苯氧基)-苯基}丙烷、雙(3,5-二甲基-4-馬來醯亞胺苯基)甲烷、雙(3-乙基-5-甲基-4-馬來醯亞胺苯基)甲烷、雙(3,5-二乙基-4-馬來醯亞胺苯基)甲烷、下式(6)表示之馬來醯亞胺化合物、該等馬來醯亞胺化合物之預聚物、或馬來醯亞胺化合物與胺化合物之預聚物。可使用該等中之1種,亦可將2種以上適當混合使用。
其中,雙(4-馬來醯亞胺苯基)甲烷、2,2-雙{4-(4-馬來醯亞胺苯氧基)-苯基}丙烷、雙(3-乙基-5-甲基-4-馬來醯亞胺苯基)甲烷、下式(6)表示之馬來醯亞胺化合物為較佳,尤其下式(6)表示之馬來醯亞胺化合物為較佳。藉由包含如此之馬來醯亞胺化合物,獲得之硬化物的耐熱性及彈性模量維持率有更加優異的傾向。 [化10]式(6)中,R5
各自獨立地表示氫原子或甲基,其中,氫原子為較佳。又,式中,n1
表示1以上之整數。n1
的上限值宜為10較佳,7更佳。
本實施形態之樹脂組成物中,就馬來醯亞胺化合物之含量而言,宜如後述般根據任意含有之經烯基取代之納迪克醯亞胺之官能基之一的烯基數(α)與馬來醯亞胺化合物之馬來醯亞胺基數(β)的官能基數之比([β/α])決定較佳。又,馬來醯亞胺化合物之含量相對於樹脂組成物中之構成樹脂之成分(亦包括藉由聚合而形成樹脂之成分。以下同樣。)之合計100質量份宜為15~70質量份較佳,20~45質量份更佳。藉由馬來醯亞胺化合物之含量為該等範圍內,可獲得即使填充無機填充材時成形性亦優異,且硬化性、及硬化時的如於例如250℃之彎曲彈性模量、焊料回流溫度下之彎曲彈性模量之熱時彈性模量優異的樹脂組成物等,且可獲得耐除膠渣性及耐化學性優異的印刷電路板等。
本實施形態之樹脂組成物,為了提高馬來醯亞胺化合物與無機填充材的黏合性,係包含苯乙烯基系矽烷化合物。苯乙烯基系矽烷化合物只要具有苯乙烯骨架與水解性基或苯乙烯骨架與羥基的矽烷化合物即可,並無特別限定,可為用作具有苯乙烯骨架與水解性基或苯乙烯骨架與羥基的矽烷偶聯劑者(所謂的苯乙烯基系矽烷偶聯劑)。苯乙烯基系矽烷化合物,以更加有效且確實地發揮本發明之作用效果的觀點觀之,宜包含下式(A)表示之化合物較佳。 [化11]此處,式(A)中,R8
表示水解性基或羥基,R9
表示氫原子或碳數1~3之烷基,R8
或R9
為多數個時,多數個R8
或R9
彼此可相同也可不同,k表示1~3之整數。作為水解性基,例如,可列舉甲氧基、乙氧基及丙氧基等烷氧基、以及氯原子及碘原子等鹵素原子(以下同樣。)。
苯乙烯基系矽烷化合物之具體例,可列舉對苯乙烯基三甲氧基矽烷、對苯乙烯基三乙氧基矽烷、對苯乙烯基甲基二甲氧基矽烷、對苯乙烯基甲基二乙氧基矽烷、及N-(乙烯基苄基)-2-胺基乙基-3-胺基丙基三甲氧基矽烷鹽酸鹽,該等中,對苯乙烯基三甲氧基矽烷、及對苯乙烯基三乙氧基矽烷為較佳,對苯乙烯基三甲氧基矽烷為更佳。作為市售品,例如,可列舉KBM-575、及KBM-1403(均為信越化學工業公司製製品名)。苯乙烯基系矽烷化合物可1種單獨使用,亦可將2種以上組合使用。
本實施形態之樹脂組成物中,苯乙烯基系矽烷化合物之含量並無特別限定,相對於樹脂組成物中之構成樹脂之成分之合計100質量份宜為0.1~15質量份較佳,0.1~10質量份更佳,0.5~5質量份特佳。藉由苯乙烯基系矽烷化合物之含量為上述範圍內,耐除膠渣性、耐化學性及絕緣可靠性進一步改善,另一方面,可進一步抑制成形性的降低。
本實施形態之樹脂組成物包含無機填充材。無機填充材有助於印刷電路板的低熱膨脹化、彈性模量、熱傳導率的改善。無機填充材只要是具有絕緣性者即可,並無特別限定,例如,可列舉天然二氧化矽、熔融二氧化矽、非晶二氧化矽及中空二氧化矽等二氧化矽類;氧化鋁、氮化鋁、氮化硼、軟水鋁石、氧化鉬、氧化鈦、矽酮橡膠、矽酮複合粉末、硼酸鋅、錫酸鋅、黏土、高嶺土、滑石、煅燒黏土、煅燒高嶺土、煅燒滑石、雲母、玻璃短纖維(E玻璃、D玻璃等玻璃微粉末類)、中空玻璃、及球狀玻璃。無機填充材可1種單獨使用,亦可將2種以上組合使用。該等中,以實現更低的熱膨脹性的觀點觀之,二氧化矽為較佳,以實現更高的熱傳導性的觀點觀之,氧化鋁及氮化鋁為較佳。又,該等無機填充材亦可為預先以苯乙烯基系矽烷化合物進行表面處理者。該表面處理的方法並無特別限定。例如,直接處理法可列舉乾式處理法及使用漿體之處理法(濕式法)等,以處理的均勻性的觀點觀之,濕式法為較佳。又,無機填充材亦可為市售的表面處理完畢之無機填充材(填料)。
本實施形態之樹脂組成物中,無機填充材之含量並無特別限定,相對於樹脂組成物中之構成樹脂之成分之合計100質量份宜為100~1100質量份較佳,100~700質量份更佳。藉由無機填充材之含量為上述範圍內,可更加良好地展現低熱膨脹化、高彈性化、及熱傳導率等無機填充材所特有的特性,另一方面可進一步抑制成形性的降低。
無機填充材的平均粒徑(D50)並無特別限定,以可形成更加微細之配線的觀點觀之,宜為0.2~10μm較佳,2~5μm更佳。又,無機填充材的粒子形狀亦無特別限定,以成形性的觀點觀之,宜為球狀或大致球狀較佳。此處,D50係指中值粒徑(median徑),係將測得之粉體之粒度分布分成2部分時較大側與較小側的質量為等量時的粒徑。一般而言可利用濕式雷射繞射・散射法測定。
本實施形態之樹脂組成物,以更加有效且確實地發揮本發明之作用效果的觀點觀之,宜包含經烯基取代之納迪克醯亞胺較佳。經烯基取代之納迪克醯亞胺只要是於分子中具有1個以上之經烯基取代之納迪克醯亞胺基的化合物即可,並無特別限定。其具體例可列舉下式(1)表示之化合物。 [化12]式(1)中,R1
各自獨立地表示氫原子、碳數1~6之烷基, R2
表示碳數1~6之伸烷基、伸苯基、伸聯苯基、伸萘基、或下式(2)或(3)表示之基。 [化13]式(2)中,R3
表示亞甲基、異亞丙基、CO、O、S、或SO2
表示之取代基。 [化14]式(3)中,R4
各自獨立地表示選出的碳數1~4之伸烷基、或碳數5~8之環伸烷基。
又,式(1)表示之經烯基取代之納迪克醯亞胺亦可使用市售品。市售品並無特別限定,例如,可列舉下式(4)表示之化合物(BANI-M(丸善石油化學(股)製))、及下式(5)表示之化合物(BANI-X(丸善石油化學(股)製))。可使用該等中之1種,亦可將2種以上組合使用。 [化15][化16]
本實施形態之樹脂組成物中,經烯基取代之納迪克醯亞胺之含量,宜如後述般根據其官能基之一的烯基與馬來醯亞胺化合物之馬來醯亞胺基的官能基數之比決定較佳。又,經烯基取代之納迪克醯亞胺之含量相對於樹脂組成物中之構成樹脂之成分之合計100質量份宜為20~50質量份較佳,25~45質量份更佳。藉由經烯基取代之納迪克醯亞胺之含量為該等範圍內,可獲得即使填充無機填充材時成形性、硬化性、及硬化時之熱時彈性模量亦優異的樹脂組成物等,且可獲得耐除膠渣性及耐化學性優異的印刷電路板等。
本實施形態之樹脂組成物中,經烯基取代之納迪克醯亞胺及馬來醯亞胺化合物之含量宜分別根據指定的官能基數之比決定較佳。此處,指定的經烯基取代之納迪克醯亞胺之官能基係鍵結於分子末端的烯基,馬來醯亞胺化合物的官能基係馬來醯亞胺基。
本實施形態之樹脂組成物,宜以滿足下式(B)表示之關係的方式包含經烯基取代之納迪克醯亞胺與馬來醯亞胺化合物較佳,以滿足下式(B1)表示之關係的方式包含更佳。 0.9≦β/α≦4.3 (B) 1.5≦β/α≦4.0 (B1) 此處,式中,α表示樹脂組成物中之經烯基取代之納迪克醯亞胺具有之烯基的總數,β表示樹脂組成物中之馬來醯亞胺化合物具有之馬來醯亞胺基的總數。藉由該官能基之比(β/α)為該等範圍內,可獲得硬化時之熱時彈性模量及易硬化性更加優異的樹脂組成物等,且可獲得低熱膨脹、耐熱性、吸濕耐熱性、耐除膠渣性及耐化學性優異的印刷電路板等。
本實施形態之樹脂組成物,除上述各成分外,宜進一步包含氰酸酯化合物較佳。藉由使用氰酸酯化合物,可獲得成形性優異的樹脂組成物、預浸體、樹脂片、覆金屬箔疊層板及印刷電路板,並可獲得金屬箔剝離強度更加優異的覆金屬箔疊層板及印刷電路板。氰酸酯化合物可1種單獨使用,亦可將2種以上組合使用。
本實施形態所使用之氰酸酯化合物的種類並無特別限定,例如可列舉下式(7)表示之萘酚芳烷基型氰酸酯、下式(8)表示之酚醛清漆型氰酸酯、聯苯芳烷基型氰酸酯、雙(3,3-二甲基-4-氰氧基苯基)甲烷、雙(4-氰氧基苯基)甲烷、1,3-二氰氧基苯、1,4-二氰氧基苯、1,3,5-三氰氧基苯、1,3-二氰氧基萘、1,4-二氰氧基萘、1,6-二氰氧基萘、1,8-二氰氧基萘、2,6-二氰氧基萘、2,7-二氰氧基萘、1,3,6-三氰氧基萘、4,4’-二氰氧基聯苯、雙(4-氰氧基苯基)醚、雙(4-氰氧基苯基)硫醚、雙(4-氰氧基苯基)碸、及2,2-雙(4-氰氧基苯基)丙烷。
其中,下式(7)表示之萘酚芳烷基型氰酸酯、下式(8)表示之酚醛清漆型氰酸酯、及聯苯芳烷基型氰酸酯,考量阻燃性優異、硬化性高、且硬化物之熱膨脹係數低的方面為特佳。
[化17]此處,式中,R6
各自獨立地表示氫原子或甲基,其中,氫原子為較佳。又,式中,n2
表示1以上之整數。n2
的上限值宜為10較佳,6更佳。 [化18]此處,式中,R7
各自獨立地表示氫原子或甲基,其中,氫原子為較佳。又,式中,n3
表示1以上之整數。n3
的上限值宜為10較佳,7更佳。
該等氰酸酯化合物的製法並無特別限定,可利用就氰酸酯合成法現有之任意方法進行製造。具體例示的話,可藉由使下式(9)表示之萘酚芳烷基型苯酚樹脂與鹵化氰於鈍性有機溶劑中在鹼性化合物存在下反應而獲得。又,亦可採取於含有水之溶液中形成同樣的萘酚芳烷基型苯酚樹脂與鹼性化合物的鹽後,進行與鹵化氰的2相系界面反應並合成的方法。
又,萘酚芳烷基型氰酸酯可選自於使藉由α-萘酚或β-萘酚等萘酚類與對苯二甲醇、α,α'-二甲氧基-對二甲苯、1,4-二(2-羥基-2-丙基)苯等之反應獲得的萘酚芳烷基樹脂和氰酸縮合而得者。
本實施形態之樹脂組成物中,氰酸酯化合物之含量並無特別限定,相對於樹脂組成物中之構成樹脂之成分之合計100質量份宜為0.01~40質量份較佳,0.01~25質量份更佳。藉由氰酸酯化合物之含量為該等範圍內,可獲得填充無機填充材時之成形性更加優異、硬化時之熱時彈性模量優異的樹脂組成物、預浸體及樹脂片,且可獲得耐除膠渣性及耐化學性更加優異的覆金屬箔疊層板及印刷電路板。
又,本實施形態之樹脂組成物中,在不損及所期望之特性的範圍內,亦可添加上述以外的樹脂(以下,有時稱為「其他樹脂」)。關於該其他樹脂的種類,只要是具有絕緣性者即可,並無特別限定,例如,可列舉環氧樹脂、苯并 化合物、苯酚樹脂、熱塑性樹脂、矽酮樹脂等樹脂。藉由適當倂用該等樹脂,可賦予預浸體及樹脂片金屬黏合性,且可賦予印刷電路板等應力緩和性。
本實施形態之樹脂組成物,為了提高無機填充材的分散性、樹脂與無機填充材、玻璃布的接著強度,亦可包含除苯乙烯基系矽烷化合物以外之具有相對於有機基形成化學鍵之基和水解性基或羥基的矽烷化合物(以下,稱為「其他矽烷化合物」。)及/或濕潤分散劑。其他矽烷化合物可為一般無機物之表面處理所使用之矽烷偶聯劑,並無特別限定。作為其他矽烷化合物之具體例,可列舉γ-胺基丙基三乙氧基矽烷、N-β-(胺基乙基)-γ-胺基丙基三甲氧基矽烷等具有胺基與水解性基或羥基的胺基系矽烷化合物;3-環氧丙氧丙基三甲氧基矽烷等具有環氧基與水解性基或羥基的環氧系矽烷化合物、γ-甲基丙烯醯氧丙基三甲氧基矽烷等具有乙烯基與水解性基或羥基的乙烯基系矽烷化合物、陽離子系矽烷偶聯劑。該等可1種單獨使用,亦可將2種以上組合使用。
上述矽烷化合物中,以進一步提高成形性的觀點觀之,宜為環氧系矽烷化合物較佳。環氧系矽烷化合物可為具有環氧基與水解性基或羥基的環氧系矽烷偶聯劑,例如,可列舉3-環氧丙氧丙基三甲氧基矽烷、3-環氧丙氧丙基甲基二甲氧基矽烷、3-環氧丙氧丙基三乙氧基矽烷、3-環氧丙氧丙基甲基二乙氧基矽烷,3-環氧丙氧丙基三甲氧基矽烷為較佳。
本實施形態之樹脂組成物中,其他矽烷化合物之含量並無特別限定,相對於樹脂組成物中之構成樹脂之成分之合計100質量份宜為0.1~15質量份較佳,0.5~5質量份更佳。藉由其他矽烷化合物之含量為該等範圍內,可獲得填充無機填充材時之成形性及硬化時之熱時彈性模量更加優異的樹脂組成物、預浸體及樹脂片,且可獲得耐除膠渣性及耐化學性更加優異的覆金屬箔疊層板及印刷電路板。
又,濕潤分散劑只要是使用於塗料用之分散穩定劑即可,並無特別限定。濕潤分散劑的市售品,例如,可列舉BYK Japan(股)製的Disperbyk-110、111、118、180、161、2009、BYK-W996、W9010、W903(均為製品名)。該等可1種單獨使用,亦可將2種以上組合使用。
又,本實施形態之樹脂組成物,在不損及所期望之特性的範圍內,亦可倂用硬化促進劑。就硬化促進劑而言,例如,可列舉咪唑化合物;過氧化苯甲醯、過氧化月桂醯、過氧化乙醯、過氧化對氯苯甲醯、二過氧鄰苯二甲酸二第三丁酯等所例示之有機過氧化物;偶氮雙腈等偶氮化合物;N,N-二甲基苄胺、N,N-二甲基苯胺、N,N-二甲基甲苯胺、2-N-乙基苯胺基乙醇、三正丁胺、吡啶、喹啉、N-甲基啉、三乙醇胺、三乙二胺、四甲基丁二胺、N-甲基哌啶等三級胺類;苯酚、二甲酚、甲酚、間苯二酚、兒茶酚等苯酚類;環烷酸鉛、硬脂酸鉛、環烷酸鋅、辛酸鋅、油酸錫、蘋果酸二丁基錫、環烷酸錳、環烷酸鈷、乙醯基丙酮鐵等有機金屬鹽;該等有機金屬鹽溶解於苯酚、雙酚等含羥基之化合物而成者;氯化錫、氯化鋅、氯化鋁等無機金屬鹽;二辛基氧化錫、其他烷基錫、烷基氧化錫等有機錫化合物等。該等可1種單獨使用,亦可將2種以上倂用。
就本實施形態之樹脂組成物而言,宜進一步含有上述硬化促進劑中之咪唑化合物較佳。咪唑化合物並無特別限定,以更加有效且確實地發揮本發明之作用效果的觀點觀之,宜為下式(11)表示之咪唑化合物較佳。 [化20]此處,式中,Ar表示苯基、萘基、聯苯基或蒽基或將該等以羥基進行改性而得之1價基,其中,苯基為較理想。R11
表示氫原子、或烷基或將其以羥基進行改性而得之1價基、或芳基,作為上述芳基,例如,可列舉經取代或未經取代之苯基、萘基、聯苯基或蒽基,苯基為較佳,Ar基及R11
基兩者均為苯基更佳。
就咪唑化合物而言,例如,可列舉2-甲基咪唑、2-乙基-4-甲基咪唑、2-苯基咪唑、1-氰基乙基-2-苯基咪唑、1-氰基乙基-2-乙基-4-甲基咪唑、2-苯基-4,5-二羥基甲基咪唑、2-苯基-4-甲基-5-羥基甲基咪唑、2,4,5-三苯基咪唑、及2-苯基-4-甲基咪唑。該等中,2,4,5-三苯基咪唑、及2-苯基-4-甲基咪唑為更佳,2,4,5-三苯基咪唑特佳。
本實施形態之樹脂組成物中,咪唑化合物之含量並無特別限定,相對於樹脂組成物中之構成樹脂之成分之合計100質量份宜為0.01~10質量份較佳,0.1~5質量份更佳。藉由咪唑化合物之含量為該等範圍內,可獲得硬化性與成形性優異的樹脂組成物、預浸體及樹脂片、以及將該等作為原材料之覆金屬箔疊層板及印刷電路板。
進一步,本實施形態之樹脂組成物,為了改善無機填充材等固體成分的分散性,亦可包含表面調整劑。表面調整劑只要是以往作為界面活性劑包含於樹脂組成物中者即可,並無特別限定,例如,可列舉聚二甲基矽氧烷系、及丙烯酸系。作為其市售品,例如,可列舉BYK Japan(股)製的BYK-310、330、346。表面調整劑可1種單獨使用,亦可將2種以上組合使用。
又,本實施形態之樹脂組成物視需要亦可含有溶劑。例如,使用有機溶劑的話,樹脂組成物製備時的黏度降低,操作性得到改善,同時可提高對於玻璃布的含浸性。就溶劑的種類而言,只要能溶解樹脂組成物中之樹脂的一部分或全部即可,並無特別限定。作為其具體例,例如,可列舉丙酮、甲乙酮、甲基賽珞蘇等酮類;甲苯及二甲苯等芳香族烴類;二甲基甲醯胺等醯胺類;以及丙二醇單甲醚及其乙酸酯等,但並不限定於該等。溶劑可1種單獨使用,亦可將2種以上組合使用。
本實施形態之樹脂組成物可依照常法製備。例如,宜為可獲得均勻地含有上述各成分之樹脂組成物的方法較佳。具體而言,例如,藉由將上述各成分依序摻合至溶劑,並充分攪拌,可輕易地製備本實施形態之樹脂組成物。又,苯乙烯基系矽烷化合物可與其他成分同樣摻合至樹脂組成物中,亦可取而代之或除此之外將無機填充材用苯乙烯基系矽烷化合物進行表面處理後,將表面鍵結有苯乙烯基系矽烷化合物之無機填充材和其他成分一起進行摻合,而製備樹脂組成物。將無機填充材用苯乙烯基系矽烷化合物進行表面處理的方法並無特別限定。例如,直接處理法可列舉乾式處理法及使用漿體之處理法(濕式法)等,以處理的均勻性的觀點觀之,濕式法為較佳。又,亦可使用市售的表面處理完畢之無機填充材(填料)。
製備本實施形態之樹脂組成物時,視需要可使用有機溶劑。就有機溶劑的種類而言,只要能溶解樹脂組成物中之樹脂即可,並無特別限定。其具體例如上述。製備樹脂組成物時,可進行用以使各成分均勻地溶解或分散之公知的處理(攪拌、混合、混練處理等)。例如,在使用無機填充材的情況下,當其均勻分散時,藉由使用設置有具適當攪拌能力之攪拌機的攪拌槽進行攪拌分散處理,對於樹脂組成物的分散性提高。上述攪拌、混合、混練處理,例如可使用球磨機、珠粒研磨機等以混合為目的之裝置、或公轉或自轉型混合裝置等公知的裝置而適當進行。
本實施形態之預浸體係具備基材、及含浸或塗佈於該基材之上述樹脂組成物的預浸體。預浸體的製造方法可依照常法進行,並無特別限定。例如,可藉由將本實施形態中之樹脂成分含浸或塗佈於基材後,在100~200℃乾燥機中加熱1~30分鐘等使其半硬化(B階段化),而製作本實施形態之預浸體。
樹脂組成物(包含無機填充材。)之含量並無特別限定,相對於預浸體之總量宜為30~90質量%較佳,35~85質量%更佳,40~80質量%尤佳。藉由樹脂組成物之含量為上述範圍內,成形性有進一步改善的傾向。
就基材而言並無特別限定,可根據目的用途、性能適當選擇並使用各種印刷電路板材料所使用之公知品。其具體例並無特別限定,例如可列舉E玻璃、D玻璃、S玻璃、Q玻璃、球狀玻璃、NE玻璃、L玻璃、T玻璃等玻璃纖維;石英等玻璃以外的無機纖維;聚對伸苯對苯二甲醯胺(Kevlar(註冊商標)、杜邦(股)公司製)、共聚對伸苯・3,4'氧基二伸苯・對苯二甲醯胺(Technora(註冊商標)、Teijin technoproducts(股)公司製)等全芳香族聚醯胺;2,6-羥基萘甲酸(naphthoic acid)・對羥基苯甲酸(Vectran(註冊商標)、Kuraray(股)公司製)、Zxion(註冊商標、KB SEIREN製)等的聚酯;聚對伸苯苯并雙唑(poly(p-phenylene-2, 6-benzobisoxazole))(Zylon(註冊商標)、東洋紡(股)公司製)、聚醯亞胺等有機纖維。該等中,以低熱膨脹率的觀點觀之,E玻璃、T玻璃、S玻璃、Q玻璃、及有機纖維為較佳。該等基材可1種單獨使用,亦可將2種以上倂用。
基材的形狀並無特別限定,例如,可列舉織布、不織布、粗紗、切股氈、表面氈等。織布的織法並無特別限定,例如,已知平織、斜子織、斜紋織等,可根據目的用途、性能從該等公知者中適當選擇並使用。又,可適當使用將該等進行開纖處理而得者、以如矽烷偶聯劑之矽烷化合物等進行表面處理而得的玻璃織布。基材的厚度、質量並無特別限定,通常宜使用0.01~0.3mm左右者較理想。尤其以強度與吸水性的觀點觀之,基材宜為厚度200μm以下、質量250g/m2
以下之玻璃織布較佳,宜為選自於由E玻璃、S玻璃、T玻璃及Q玻璃之玻璃纖維以及有機纖維構成之群組中之1種以上之纖維的織布(cloth)更佳。
本實施形態之樹脂片具備:支持體(基材片)、及塗佈於該基材片之上述樹脂組成物,上述樹脂組成物係疊層於該基材片之單面或兩面。樹脂片係作為薄片化的一種方式使用,例如,可於金屬箔、膜等支持體直接塗佈預浸體等所使用之熱硬化性樹脂(包含無機填充材)並乾燥而製造。
基材片並無特別限定,可使用用於各種印刷電路板材料之公知的物質。例如可列舉聚醯亞胺膜、聚醯胺膜、聚酯膜、聚對苯二甲酸乙二酯(PET)膜、聚對苯二甲酸丁二酯(PBT)膜、聚丙烯(PP)膜、聚乙烯(PE)膜、鋁箔、銅箔、金箔等。其中,電解銅箔、PET膜為較佳。
就塗佈方法而言,例如,可列舉將本實施形態之樹脂組成物溶解於溶劑而得之溶液利用桿塗機、模塗機、刮刀塗佈機、貝克塗抹機等塗佈在基材片上的方法。
就樹脂片而言,宜為將上述樹脂組成物塗佈於支持體(基材片)後,使其半硬化(B階段化)而得者較佳。具體而言,例如,可列舉以下的方法等:將上述樹脂組成物塗佈於銅箔等基材片後,藉由在100~200℃乾燥機中加熱1~60分鐘的方法等使其半硬化,而製造樹脂片。樹脂組成物於支持體之附著量,以樹脂片之樹脂厚計宜為1~300μm之範圍較佳。本實施形態之樹脂片可用作印刷電路板之堆積材料。
本實施形態之疊層板係重疊1片以上選自於由上述預浸體及樹脂片構成之群組中之至少1種而得,包括選自於由該預浸體及樹脂片構成之群組中之至少1種中所含之樹脂組成物之硬化物。該疊層板,例如,可將1片以上之選自於由上述預浸體及樹脂片構成之群組中之至少1種予以重疊並硬化而獲得。又,本實施形態之覆金屬箔疊層板,係具有選自於由上述預浸體及樹脂片構成之群組中之至少1種、以及配置在選自於由該預浸體及樹脂片構成之群組中之至少1種之單面或兩面的金屬箔,包括選自於由該預浸體及樹脂片構成之群組中之至少1種中所含之樹脂組成物之硬化物。該覆金屬箔疊層板,可藉由重疊1片以上選自於由上述預浸體及樹脂片構成之群組中之至少1種,在其單面或兩面配置金屬箔並疊層成形而獲得。更具體而言,可藉由重疊1片或多片前述預浸體及/或樹脂片,視所需在其單面或兩面配置銅、鋁等金屬箔,必要時進行疊層成形,而製造覆金屬箔疊層板。此處所使用之金屬箔只要是用於印刷電路板材料者即可,並無特別限定,宜為壓延銅箔、電解銅箔等公知的銅箔較佳。又,金屬箔的厚度並無特別限定,宜為1~70μm較佳,1.5~35μm更佳。覆金屬箔疊層板的成形方法及其成形條件亦無特別限定,可適用一般印刷電路板用疊層板及多層板的方法及條件。例如,覆金屬箔疊層板成形時可使用多段壓製機、多段真空壓製機、連續成形機、高壓釜成形機等。又,覆金屬箔疊層板成形時,溫度一般為100~300℃,壓力一般為面壓2~100kgf/cm2
,加熱時間一般為0.05~5小時之範圍。進一步,必要時亦可於150~300℃之溫度實施後硬化。又,藉由將上述預浸體和另外製作的內層用配線板予以組合並疊層成形,亦可製成多層板。
本實施形態之印刷電路板係包括絕緣層、及形成在該絕緣層之表面之導體層的印刷電路板,該絕緣層包含上述樹脂組成物。成為電路之導體層可由上述覆金屬箔疊層板中之金屬箔形成,或亦可藉由無電解鍍敷於絕緣層之表面形成。該印刷電路板係耐化學性、耐除膠渣性及絕緣可靠性優異者,可特別有效地用作要求該等性能的半導體封裝用印刷電路板。
本實施形態之印刷電路板,具體而言,例如,可利用以下之方法製造。首先,準備上述覆金屬箔疊層板(覆銅疊層板等)。對於覆金屬箔疊層板之表面施以蝕刻處理,而形成內層電路,製成內層基板。對於該內層基板之內層電路表面視需要施以用於提高接著強度之表面處理,然後,於該內層電路表面重疊所需片數的上述預浸體,進一步於其外側疊層外層電路用之金屬箔,進行加熱加壓並一體成形。以此種方式,製造於內層電路與外層電路用金屬箔之間形成有基材及由熱硬化性樹脂組成物之硬化物構成之絕緣層的多層疊層板。然後,對於該多層疊層板施以通孔、介層孔(via hole)用之開孔加工後,為了去除係來自硬化物層所含之樹脂成分之樹脂之殘渣的膠渣(smear),實施除膠渣處理。之後在該孔的壁面形成使內層電路與外層電路用金屬箔導通之鍍敷金屬皮膜,進一步對於外層電路用金屬箔施以蝕刻處理並形成外層電路,而製成印刷電路板。
例如,上述預浸體(基材及附著於該基材之上述樹脂組成物)、覆金屬箔疊層板之樹脂組成物層(由上述樹脂組成物構成之層)構成含有上述樹脂組成物之絕緣層。
本實施形態中,就絕緣層而言,於250℃之彎曲彈性模量相對於於25℃之彎曲彈性模量的比例(以下,稱為「彈性模量維持率」。)為80~100%的話,可進一步抑制加熱印刷電路板時的翹曲故較佳。使彈性模量維持率成為80~100%的方法並無特別限定,例如,可列舉將絕緣層所使用之樹脂組成物之各成分的種類及含量在上述範圍內適當調整的方法。彈性模量維持率,具體而言可利用下列方法求出。亦即,依照JIS C 6481規定之方法,利用Autograph分別於25℃、250℃測定彎曲彈性模量(彎曲強度)。由測得之25℃之彎曲彈性模量(a)與250℃之熱時彎曲彈性模量(b)依下式算出彈性模量維持率。 彈性模量維持率=(b)/(a)×100
除該方法外,只要不損害本發明之目的,亦可使用現有的方法使彈性模量維持率成為80~100%。例如,可列舉藉由導入奈米填料而限制分子運動的方法、利用溶膠-凝膠法將奈米二氧化矽混成於絕緣層使用之樹脂之交聯點的方法、或絕緣層使用之樹脂本身高Tg化、或使於400℃以下之範圍內無Tg化等方法。
又,在不使用覆金屬箔疊層板的情況下,可於上述預浸體、或上述樹脂片形成成為電路之導體層而製成印刷電路板。此時,導體層的形成可使用無電解鍍敷的方法。
關於本實施形態之印刷電路板,上述絕緣層於半導體封裝時之回流溫度下仍維持優異的彈性模量,能有效地抑制半導體塑膠封裝之翹曲,故可特別有效地用作半導體封裝用印刷電路板。 [實施例]
以下,藉由實施例對本發明進行更詳細地說明,但本發明並不限定於該等實施例。
(合成例1) α-萘酚芳烷基型氰酸酯樹脂之合成 將安裝有溫度計、攪拌器、滴加漏斗及回流冷卻器的反應器預先以滷水冷卻至0~5℃,向其中加入氯化氰7.47g(0.122mol)、35%鹽酸9.75g(0.0935mol)、水76mL、及二氯甲烷44mL。保持該反應器內之溫度為-5~+5℃、pH為1以下的狀態,於攪拌下以滴加漏斗歷時1小時滴加上式(9)中之R8
均為氫原子的α-萘酚芳烷基型苯酚樹脂(SN485、OH基當量:214g/eq.、軟化點:86℃、新日鐵化學(股)製)20g(0.0935mol)、及三乙胺14.16g(0.14mol)溶解於二氯甲烷92mL而得之溶液,滴加結束後,進一步歷時15分鐘滴加三乙胺4.72g(0.047mol)。滴加結束後,於同溫度攪拌15分鐘後將反應液分液,分取出有機層。將獲得之有機層以水100mL洗淨2次後,利用蒸發器於減壓下餾去二氯甲烷,最後於80℃進行1小時濃縮乾固,獲得α-萘酚芳烷基型苯酚樹脂之氰酸酯化物(α-萘酚芳烷基型氰酸酯樹脂、官能基當量:261g/eq.)23.5g。
(實施例1) 於合成例1獲得之α-萘酚芳烷基型氰酸酯樹脂10質量份、酚醛清漆型馬來醯亞胺化合物(BMI-2300、大和化成工業(股)製、官能基當量:186g/eq.)45質量份、及雙烯丙基納迪克醯亞胺(BANI-M、丸善石油化學(股)製、官能基當量:286g/eq.)45質量份,混合球狀二氧化矽(SC-5050MOB、粒徑1.6μm、Admatechs(股)公司製)150質量份、係環氧系矽烷化合物之3-環氧丙氧丙基三甲氧基矽烷(KBM-403、信越化學工業(股)製)2.5質量份、係苯乙烯基系矽烷化合物之對苯乙烯基三甲氧基矽烷(KBM-1403、信越化學工業(股)製)2.5質量份、及濕潤分散劑(DISPERBYK-161、BYK Japan(股)製)1質量份,並以甲乙酮進行稀釋獲得清漆。將該清漆含浸塗覆於E玻璃織布,在160℃加熱乾燥3分鐘,獲得樹脂組成物含量49質量%之預浸體。此時[β/α]為1.54。此處,[β/α]係以下列計算式表示(以下同樣。)。 [β/α]=(馬來醯亞胺化合物之質量份數/馬來醯亞胺化合物之官能基當量)/(經烯基取代之納迪克醯亞胺之質量份數/經烯基取代之納迪克醯亞胺之官能基當量)
(實施例2) 使用係苯乙烯基系矽烷化合物之對苯乙烯基三甲氧基矽烷(KBM-1403、信越化學工業(股)製)5質量份替換係環氧系矽烷化合物之3-環氧丙氧丙基三甲氧基矽烷(KBM-403、信越化學工業(股)製)2.5質量份、及係苯乙烯基系矽烷化合物之對苯乙烯基三甲氧基矽烷(KBM-1403、信越化學工業(股)製)2.5質量份,除此以外,與實施例1同樣進行獲得清漆,並與實施例1同樣進行獲得預浸體。
(比較例1) 使用係環氧系矽烷化合物之3-環氧丙氧丙基三甲氧基矽烷(KBM-403、信越化學工業(股)製)5質量份替換係環氧系矽烷化合物之3-環氧丙氧丙基三甲氧基矽烷(KBM-403、信越化學工業(股)製)2.5質量份、及係苯乙烯基系矽烷化合物之對苯乙烯基三甲氧基矽烷(KBM-1403、信越化學工業(股)製)2.5質量份,除此以外,與實施例1同樣進行獲得清漆,並與實施例1同樣進行獲得預浸體。
(比較例2) 使用係丙烯酸系矽烷化合物之3-丙烯醯氧丙基三甲氧基矽烷(KBM-5103、信越化學工業(股)製)5質量份替換係環氧系矽烷化合物之3-環氧丙氧丙基三甲氧基矽烷(KBM-403、信越化學工業(股)製)2.5質量份、及係苯乙烯基系矽烷化合物之對苯乙烯基三甲氧基矽烷(KBM-1403、信越化學工業(股)製)2.5質量份,除此以外,與實施例1同樣進行獲得清漆,並與實施例1同樣進行獲得預浸體。
(比較例3) 使用係環氧系矽烷化合物之3-環氧丙氧丙基三甲氧基矽烷(KBM-403、信越化學工業(股)製)2.5質量份、及係丙烯酸系矽烷化合物之3-丙烯醯氧丙基三甲氧基矽烷(KBM-5103、信越化學工業(股)製)2.5質量份替換係環氧系矽烷化合物之3-環氧丙氧丙基三甲氧基矽烷(KBM-403、信越化學工業(股)製)2.5質量份、及係苯乙烯基系矽烷化合物之對苯乙烯基三甲氧基矽烷(KBM-1403、信越化學工業(股)製)2.5質量份,除此以外,與實施例1同樣進行獲得清漆,並與實施例1同樣進行獲得預浸體。
(比較例4) 使用係烯烴系矽烷化合物之辛烯基三甲氧基矽烷(KBM-1083、信越化學工業(股)製)5質量份替換係環氧系矽烷化合物之3-環氧丙氧丙基三甲氧基矽烷(KBM-403、信越化學工業(股)製)2.5質量份、及係苯乙烯基系矽烷化合物之對苯乙烯基三甲氧基矽烷(KBM-1403、信越化學工業(股)製)2.5質量份,除此以外,與實施例1同樣進行獲得清漆,並與實施例1同樣進行獲得預浸體。
(比較例5) 使用係丙烯酸系矽烷化合物之甲基丙烯醯氧辛基三甲氧基矽烷(KBM-5803、信越化學工業(股)製)5質量份替換係環氧系矽烷化合物之3-環氧丙氧丙基三甲氧基矽烷(KBM-403、信越化學工業(股)製)2.5質量份、及係苯乙烯基系矽烷化合物之對苯乙烯基三甲氧基矽烷(KBM-1403、信越化學工業(股)製)2.5質量份,除此以外,與實施例1同樣進行獲得清漆,並與實施例1同樣進行獲得預浸體。
[覆金屬箔疊層板的製作] 將上述獲得之預浸體各重疊1片、4片、8片,並在上下配置12μm厚之電解銅箔(3EC-III、三井金屬礦業(股)製),以壓力30kgf/cm2
、溫度220℃進行120分鐘的疊層成型,獲得絕緣層厚度0.1mm、0.4mm、0.8mm的覆銅疊層板作為覆金屬箔疊層板。
[絕緣可靠性] 絕緣可靠性係藉由利用HAST(高加速壽命試驗)所為之線間絕緣可靠性試驗進行評價。首先,由上述獲得之覆銅疊層板(厚度0.1mm)利用減成(subtractive)法形成印刷電路板(L/S=100/100μm)。然後,將配線連接電源,於溫度130℃、濕度85%、施加電壓5VDC之條件下評價連續濕中絕緣電阻。此外,電阻值1.0×108
Ω以下判定為故障。評價基準如下。 ○:500小時以上無故障 ×:未達500小時已有故障 結果顯示於表1中。
[耐化學性] 將覆銅疊層板(50mm×50mm×0.4mm)於已調整至1N的70℃氫氧化鈉水溶液中浸漬2小時。由浸漬前後之覆銅疊層板之質量算出重量減少量(質量%)。絕對值越低,越顯示優異的耐化學性(耐鹼性)。結果顯示於表1中。
[耐除膠渣性] 將覆銅疊層板(50mm×50mm×0.4mm)之兩面的銅箔利用蝕刻去除後,在80℃於係膨潤液之Atotech Japan(股)之Swelling Dip Securiganth P中浸漬10分鐘,然後在80℃於係粗化液之Atotech Japan(股)之Concentrate compact CP中浸漬5分鐘,最後在45℃於係中和液之Atotech Japan(股)之Reduction conditioner Securiganth P500中浸漬10分鐘。重複3次該處理。由處理前後之覆銅疊層板之質量測得質量減少量(質量%)。絕對值越低,越顯示優異的耐除膠渣性。結果顯示於表1中。
[彈性模量維持率] 使用將銅箔從覆銅疊層板(50mm×25mm×0.8mm)之兩面剝離而獲得之樣品,依照JIS C-6481,利用Autograph(島津製作所(股)製AG-Xplus)分別測定25℃、250℃之彎曲彈性模量。由利用上述方法測得之25℃之彎曲彈性模量(a)與250℃之彎曲彈性模量(b),依下式算出彈性模量維持率。 彈性模量維持率=(b)/(a)×100
[耐熱性] 使覆銅疊層板(50mm×25mm×0.4mm)於280℃之焊料中流動30分鐘,目視確認有無分層,而評價耐熱性。評價基準如下。 ○:沒有任何異常 ×:使其流動0~30分鐘期間發生分層
本申請案係基於2015年7月6日提申的日本專利申請案(日本特願2015-135212),其內容在此納入作為參考。 [產業上利用性]
根據本發明可提供一種印刷電路板用絕緣層,該印刷電路板用絕緣層不僅是耐化學性、耐除膠渣性及絕緣可靠性優異,耐熱性及彈性模量損失率亦優異,故在用於半導體塑膠封裝之印刷電路板等領域具有產業利用性。
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Claims (17)
- 一種樹脂組成物,包括馬來醯亞胺化合物、具有苯乙烯骨架與水解性基或苯乙烯骨架與羥基之矽烷化合物、無機填充材、以及經烯基取代之納迪克醯亞胺。
- 如申請專利範圍第1或2項之樹脂組成物,更包括氰酸酯化合物。
- 如申請專利範圍第1或2項之樹脂組成物,其中,該無機填充材係預先利用該矽烷化合物進行了表面處理。
- 如申請專利範圍第1或2項之樹脂組成物,其中,該矽烷化合物之含量相對於樹脂組成物中之構成樹脂之成分之合計100質量份為0.1~15質量份。
- 如申請專利範圍第1或2項之樹脂組成物,其中,該無機填充材包括選自於由二氧化矽、氧化鋁及氮化鋁構成之群組中之至少1種。
- 如申請專利範圍第1或2項之樹脂組成物,其中,該無機填充材之含量相對於樹脂組成物中之構成樹脂之成分之合計100質量份為100~1100質量份。
- 一種預浸體,具備:基材,及含浸或塗佈於該基材之如申請專利範圍第1至11項中任一項之樹脂組成物。
- 如申請專利範圍第12項之預浸體,其中,該基材係選自於由E玻璃布、T玻璃布、S玻璃布、Q玻璃布及有機纖維布構成之群組中之至少1種。
- 一種樹脂片,具備:支持體,及塗佈於該支持體之如申請專利範圍第1至11項中任一項之樹脂組成物。
- 一種疊層板,係重疊1片以上選自於由如申請專利範圍第12及13項之預浸體、及如申請專利範圍第14項之樹脂片構成之群組中之至少1種而得,包括選自於由該預浸體及該樹脂片構成之群組中之至少1種中所含之樹脂組成物之硬化物。
- 一種覆金屬箔疊層板,具有:選自於由如申請專利範圍第12及13項之預浸體、及如申請專利範圍第14項之樹脂片構成之群組中之至少1種,以及配置在選自於由該預浸體及該樹脂片構成之群組中之至少1種之單面或兩面的金屬箔;包括選自於由該預浸體及該樹脂片構成之群組中之至少1種中所含之樹脂組成物之硬化物。
- 一種印刷電路板,包括絕緣層及形成在該絕緣層之表面之導體層,該絕緣層包括如申請專利範圍第1至11項中任一項之樹脂組成物。
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- 2016-07-04 JP JP2017527444A patent/JP6732215B2/ja active Active
- 2016-07-06 TW TW105121325A patent/TWI698466B/zh active
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2020
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- 2020-07-07 JP JP2020117116A patent/JP2020176267A/ja active Pending
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2021
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KR102579981B1 (ko) | 2023-09-18 |
US11195638B2 (en) | 2021-12-07 |
JP2020176267A (ja) | 2020-10-29 |
KR20180027418A (ko) | 2018-03-14 |
WO2017006896A1 (ja) | 2017-01-12 |
CN107849361B (zh) | 2020-10-16 |
EP3321326A1 (en) | 2018-05-16 |
EP3321326A4 (en) | 2019-02-27 |
CN107849361A (zh) | 2018-03-27 |
US20220076859A1 (en) | 2022-03-10 |
US20180197655A1 (en) | 2018-07-12 |
TW201706338A (zh) | 2017-02-16 |
US11769607B2 (en) | 2023-09-26 |
EP3321326B1 (en) | 2020-02-19 |
JP6732215B2 (ja) | 2020-07-29 |
US20200152349A1 (en) | 2020-05-14 |
JPWO2017006896A1 (ja) | 2018-04-19 |
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