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TWI642151B - 預浸體、覆金屬積層板及印刷配線板 - Google Patents

預浸體、覆金屬積層板及印刷配線板 Download PDF

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Publication number
TWI642151B
TWI642151B TW106112886A TW106112886A TWI642151B TW I642151 B TWI642151 B TW I642151B TW 106112886 A TW106112886 A TW 106112886A TW 106112886 A TW106112886 A TW 106112886A TW I642151 B TWI642151 B TW I642151B
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TW
Taiwan
Prior art keywords
resin
prepreg
mass
component
cured product
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TW106112886A
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English (en)
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TW201739019A (zh
Inventor
小畑心平
高橋龍史
星野泰範
Original Assignee
日商松下知識產權經營股份有限公司
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Publication of TW201739019A publication Critical patent/TW201739019A/zh
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Abstract

預浸體具備強化纖維基材及浸潤在強化纖維基材中之樹脂組成物的半硬化物。硬化後，玻璃轉移溫度(Tg)為150℃以上且220℃以下。樹脂組成物含有(A)熱硬化性樹脂，及(B)選自內核外殼橡膠(core shell rubber)與重量平均分子量為10萬以上之高分子成分中的至少1種。相對於(A)成分100質量份，(B)成分含量為30質量份以上且100質量份以下。

Description

預浸體、覆金屬積層板及印刷配線板
發明領域 本發明涉及一種預浸體、覆金屬積層板及印刷配線板。
發明背景 印刷配線板已廣泛使用在電子機器、通訊機器、計算機等各種領域。近年，尤其是攜帶式通訊終端或筆記型PC等小型可攜式機器的多機能化、高性能化、薄型化･小型化進展神速。隨之而來的，使用於該等產品的印刷配線板也追求導體配線之微細化、導體配線層之多層化、薄型化、機械特性等高性能化。尤其，隨著印刷配線板薄型化進步，有印刷配線板上搭載有半導體晶片之半導體封裝件發生翹曲而容易發生安裝不良的問題。
為了抑制印刷配線板上搭載有半導體晶片之半導體封裝件翹曲，專利文獻1中揭示了一種覆金屬積層板，其在含有環氧樹脂組成物及纖維基材之絕緣層兩面具有金屬箔，其中，環氧樹脂組成物含有環氧樹脂、雙馬來亞醯胺化合物及無機充填材，且覆金屬積層板在30℃至260℃範圍內的尺寸變化之遲滯(hysteresis)程度在預定範圍內。文獻中指出，該環氧樹脂組成物含有雙馬來亞醯胺化合物且上述遲滯程度在預定範圍內，所以即使發生了超過絕緣層之玻璃轉移溫度的巨大溫度變化，絕緣層之平面方向(XY方向)在30~260℃範圍內所算出的平均線膨脹係數很小，可減低印刷配線板上搭載有半導體元件之半導體裝置在常溫(23℃)及260℃下的翹曲量。
然而，專利文獻1中記載之覆金屬積層板卻有無法充分控制半導體封裝件翹曲的問題。
又，在印刷配線板，為了使不同層之導體圖案彼此行層連接，常利用鑽孔加工或雷射加工進行穿孔。穿孔時，會於孔內壁產生樹脂膠渣(smear)。所以，需要進行用以去除這類樹脂膠渣的除膠渣(desmear)處理。除膠渣處理譬如可使用過錳酸鉀等過錳酸鹽進行。
然而，經除膠渣處理除去之樹脂膠渣的量(除膠渣蝕刻量)一多，即可能發生孔變形或銅箔剝離等，恐降低印刷配線板之導通可靠性。所以，也講求減少除膠渣蝕刻量，亦即除膠渣耐性須佳。 先前技術文獻
專利文獻 專利文獻1：日本特開2015-63040號公報
發明概要 本發明目的在於提供一種即使印刷配線板厚度很薄，也可減少因溫度變化所造成的半導體封裝件翹曲量，同時除膠渣耐性優異的預浸體、覆金屬積層板及印刷配線板。
本發明之一態樣之預浸體的特徵在於，具備強化纖維基材及含浸在前述強化纖維基材中之樹脂組成物的半硬化物，且硬化後玻璃轉移溫度(Tg)為150℃以上且220℃以下；前述樹脂組成物含有(A)熱硬化性樹脂、及(B)選自內核外殼橡膠與重量平均分子量為10萬以上之高分子成分中的至少1種；相對於前述(A)成分100質量份，前述(B)成分之含量為30質量份以上且100質量份以下。
本發明之一態樣之覆金屬積層板的特徵在於具備一片前述預浸體的硬化物或多片前述預浸體之積層物的硬化物，及接著在前述硬化物之單面或雙面的金屬箔。
本發明之一態樣之印刷配線板的特徵在於具備一片前述預浸體的硬化物或多片前述預浸體之積層物的硬化物，及設置在前述硬化物之單面或雙面的金屬箔。
用以實施發明之形態 以下說明本發明之實施形態。 [預浸體]
本實施形態之預浸體(以下有時僅稱預浸體)具備強化纖維基材及浸潤在強化纖維基材中之樹脂組成物的半硬化物，且硬化後玻璃轉移溫度(Tg)為150℃以上且220℃以下。樹脂組成物含有(A)熱硬化性樹脂，及(B)選自內核外殼橡膠(以下有時稱內核外殼橡膠(B1))及重量平均分子量為10萬以上之高分子成分(以下有時僅稱高分子成分(B2))中的至少1種(以下有時僅稱橡膠成分(B))。相對於(A)成分100質量份，橡膠成分(B)((B)成分)含量為30質量份以上且100質量份以下。將本實施形態之預浸體作為印刷配線板上搭載有半導體晶片之半導體封裝件的材料使用時，無須以預浸體之硬化物的熱膨脹係數在預定範圍內且提高預浸體之硬化物在260℃下之彈性係數的方式來調整樹脂組成物，也能有效緩和半導體晶片與印刷配線板上所產生的應力，從而減少因溫度變化所致半導體封裝件之翹曲量。此外，將本實施形態之預浸體用於印刷配線板時，可減少為了層連接而進行穿孔時產生的樹脂膠渣之除膠渣蝕刻量，便不易降低印刷配線板的導通可靠性。
預浸體之硬化物的玻璃轉移溫度(Tg)為150℃以上且220℃以下，宜為160℃以上且200℃以下，較宜為180℃以上且200℃以下。預浸體之硬化物的玻璃轉移溫度(Tg)若超過220℃，因溫度變化所致半導體封裝件之翹曲量恐增大。又，預浸體之硬化物的玻璃轉移溫度(Tg)若低於150℃，除膠渣耐性恐不足。
預浸體之硬化物在260℃下之彈性係數宜為0.5GPa以上且7.0GPa以下，較宜為0.5GPa以上且5.0GPa以下。預浸體之硬化物在260℃下之彈性係數只要在上述範圍內，便更能縮小半導體封裝件因溫度變化所造成的翹曲量。
預浸體之厚度視雙面覆銅積層板之使用用途等所要求的特性適宜選定即可，宜為0.010~0.200mm。相對於預浸體100質量份，預浸體之樹脂含量(樹脂組成物含量)宜為30~80質量份。 [樹脂組成物之半硬化物]
樹脂組成物之半硬化物係使樹脂組成物半硬化而成。
樹脂組成物含有熱硬化性樹脂(A)及橡膠成分(B)，亦可應需求進一步含有無機充填材(C)、硬化劑、硬化促進劑、添加劑。 {熱硬化性樹脂(A)}
樹脂組成物含有熱硬化性樹脂(A)。熱硬化性樹脂(A)譬如可使用環氧樹脂、酚樹脂、雙馬來亞醯胺樹脂、氰酸酯樹脂等。可僅使用該等中之1種，亦可將該等2種以上組合使用。其中，熱硬化性樹脂(A)宜由選自於由環氧樹脂、酚樹脂、雙馬來亞醯胺樹脂及氰酸酯樹脂所構成群組中之至少1種(以下稱作熱硬化性樹脂(A1))所構成。 (環氧樹脂)
環氧樹脂可使用雙酚型環氧樹脂、酚醛型環氧樹脂、聯苯型環氧樹脂、伸茬基型環氧樹脂、芳基伸烷基型環氧樹脂、萘型環氧樹脂、萘骨架改質環氧樹脂、三苯甲烷型環氧樹脂、蒽型環氧樹脂、二環戊二烯型環氧樹脂、降莰烯型環氧樹脂、茀型環氧樹脂及將上述環氧樹脂鹵化而成的阻燃化環氧樹脂等。可僅使用該等中之1種，亦可將該等2種以上組合使用。雙酚型環氧樹脂可使用雙酚A型環氧樹脂、雙酚F型環氧樹脂、雙酚S型環氧樹脂等。酚醛型環氧樹脂可使用苯酚酚醛型環氧樹脂、甲酚酚醛型環氧樹脂等。芳基伸烷基型環氧樹脂譬如可使用苯酚芳烷基型環氧樹脂、聯苯芳烷基型環氧樹脂、聯苯酚醛型環氧樹脂、聯苯二亞甲基型環氧樹脂、三酚甲烷酚醛型環氧樹脂、四甲基聯苯型環氧樹脂等。萘骨架改質環氧樹脂譬如可使用萘骨架改質甲酚酚醛型環氧樹脂、萘二酚芳烷基型環氧樹脂、萘酚芳烷基型環氧樹脂、甲氧基萘改質甲酚酚醛型環氧樹脂、甲氧基萘二亞甲基型環氧樹脂等。
環氧樹脂之環氧當量宜為180g/eq以上，較宜為200g/eq以上。環氧當量若在上述範圍內，樹脂組成物之硬化物的交聯密度就不易變高，於是預浸體之硬化物的玻璃轉移溫度便不易超過220℃。在此，環氧當量意指每一環氧基的平均化合物質量數。羥基當量意指每一羥基的平均化合物質量數。 (酚樹脂)
酚樹脂譬如可使用聯苯芳烷基型酚樹脂、苯基芳烷基型酚樹脂、酚醛型酚樹脂、甲酚酚醛型酚樹脂、雙酚A酚醛型酚樹脂、萘型酚樹脂、四酚型酚樹脂、磷改質酚樹脂等。可僅使用該等中之1種，亦可將該等2種以上組合使用。
酚樹脂之羥基當量宜為140g/eq以上，較宜為200g/eq以上。羥基當量若在上述範圍內，樹脂組成物之硬化物的交聯密度就不易變高，於是預浸體之硬化物的玻璃轉移溫度便不易增高。 (雙馬來亞醯胺樹脂)
雙馬來亞醯胺樹脂可使用4,4'-二苯甲烷雙馬來亞醯胺、苯甲烷馬來亞醯胺、間伸苯基雙馬來醯亞胺、雙酚A二苯基醚雙馬來亞醯胺、3,3'-二甲基-5,5'-二乙基-4,4'-二苯甲烷雙馬來亞醯胺、4-甲基-1,3-伸苯基雙馬來亞醯胺、1,6'-雙馬來亞醯胺-(2,2,4-三甲基)己烷等。該等可單獨使用或可將2種以上組合使用。 (氰酸酯樹脂)
氰酸酯樹脂以1分子中具有2個以上氰酸酯基者為宜，譬如可使用2,2-雙(4-氰酸酯基苯基)丙烷(雙酚A型氰酸酯樹脂)、雙(3,5-二甲基-4-氰酸酯基苯基)甲烷、2,2-雙(4-氰酸酯基苯基)乙烷及該等之衍生物等芳香族系氰酸酯化合物等。該等可單獨使用或可將2種以上組合使用。 {橡膠成分(B)}
樹脂組成物含有選自內核外殼橡膠(B1)及重量平均分子量為10萬以上之高分子成分(B2)中的至少1種(B)。亦即，樹脂組成物可應熱硬化性樹脂(A)之成分等，於橡膠成分(B)中含有內核外殼橡膠(B1)及高分子成分(B2)，亦可僅含有內核外殼橡膠(B1)，或可僅含有高分子成分(B2)。若慮及翹曲特性與加工性(譬如雷射加工性)的平衡性，宜含有內核外殼橡膠(B1)及高分子成分(B2)。
相對於熱硬化性樹脂(A)100質量份，橡膠成分(B)含量為30質量份以上且100質量份以下。橡膠成分(B)含量超過100質量份時，如後述在製作預浸體時使用的清漆狀基底樹脂會增黏，恐無法製作預浸體。另一方面，橡膠成分(B)含量低於30質量份時，因溫度變化所致半導體封裝件之翹曲量恐增大。
橡膠成分(B)含有內核外殼橡膠(B1)及後述之丙烯酸樹脂(B2a)時，相對於熱硬化性樹脂(A)100質量份，內核外殼橡膠(B1)及丙烯酸樹脂(B2a)之含量宜為50質量份以上且100質量份以下，較宜為60質量份以上且80質量份以下。內核外殼橡膠(B1)及丙烯酸樹脂(B2a)之含量若在上述範圍內，便可進一步減少因溫度變化所致半導體封裝件之翹曲量。 (內核外殼橡膠(B1))
內核外殼橡膠(B1)係由中心部(內核相)與其周圍(外殼相)兩者不同之聚合物所構成的內核外殼型結構之橡膠成分。
構成內核相之聚合物可舉如聚矽氧/丙烯酸聚合物、丙烯酸系聚合物、聚矽氧系聚合物、丁二烯系聚合物、異戊二烯系聚合物等。構成外殼相之聚合物可舉如聚甲基丙烯酸甲酯、聚苯乙烯等。
這類的內核外殼橡膠(B1)可使用Mitsubishi Rayon Co., Ltd.製品號「S2100」、「SX-005」、「S-2001」、「S-2006」、「S-2030」、「S-2200」、「SRK200A」、「SX-006」；Aica Kogyo Co., Ltd.製品號「AC3816」、「AC3816N」、「AC3832」、「AC4030」、「AC3364」、「IM101」；KANEKA股份有限公司製「MX-217」、「MX-153」「MX-960」等。 (高分子成分(B2))
高分子成分(B2)之重量平均分子量為10萬以上，從提升成型性的觀點來看，宜為85萬以下。高分子成分(B2)之重量平均分子量低於10萬時，緩和半導體晶片與印刷配線板上所生應力的效果會不足，因溫度變化所致半導體封裝件之翹曲量恐增大。
高分子成分(B2)之材質譬如可使用丙烯酸樹脂、聚矽氧樹脂等彈性體等。可僅使用該等中之1種，亦可將2種以上組合使用。其中，高分子成分(B2)之材質又以丙烯酸樹脂為宜。藉由橡膠成分(B)含有丙烯酸樹脂，可使預浸體之硬化物低彈性化，從而可進一步減少因溫度變化所致半導體封裝件之翹曲量。
丙烯酸樹脂宜使用具有下述式(1)、(2)、(3)所示結構之丙烯酸樹脂(B2a)。 [化學式1]
x為0或大於0之整數。y為0或大於0之整數。z為0或大於0之整數。惟，排除x、y、z全部同時為0之情況。式(2)中，R1為氫原子或甲基，R2為氫原子或烷基。式(3)中，R3為氫原子或甲基，R4為選自-Ph(苯基)、-COOCH2 Ph及-COO(CH2 )2 Ph中之至少1種。
亦即，丙烯酸樹脂(B2a)之主鏈宜由前述式(1)、式(2)及式(3)中之至少前述式(2)及式(3)所示結構構成。又，丙烯酸樹脂(B2a)之分子中亦可一部分含有環氧基。
丙烯酸樹脂(B2a)之主鏈由前述式(1)、式(2)及式(3)所示結構構成時，前述式(1)、式(2)及式(3)所示結構之配列順序無特別限定。此時，丙烯酸樹脂(B2a)之主鏈上，前述式(1)所示結構彼此可連續亦可不連續，前述式(2)所示結構彼此可連續亦可不連續，並且，前述式(3)所示結構彼此可連續亦可不連續。
丙烯酸樹脂(B2a)之主鏈由前述式(2)及式(3)所示結構構成時，也不會特別限定前述式(2)及式(3)所示結構之配列順序。此時，丙烯酸樹脂(B2a)之主鏈上，前述式(2)所示結構彼此可連續亦可不連續，並且，前述式(3)所示結構彼此可連續亦可不連續。
前述式(3)所示結構亦可具有Ph(苯基)、-COOCH2 Ph及-COO(CH2 )2 Ph。丙烯酸樹脂(B2a)在碳原子間宜不具有雙鍵或三鍵等不飽和鍵。亦即，丙烯酸樹脂(B2a)之碳原子彼此宜由飽和鍵(單鍵)鍵結。丙烯酸樹脂(B2a)之重量平均分子量(Mw)宜為20萬~85萬。 (無機充填材(C))
樹脂組成物更可含有無機充填材(C)。藉由樹脂組成物含有無機充填材(C)，可達到低熱膨脹化。
無機充填材(C)之材質譬如可使用熔融二氧化矽(SiO2 )、結晶二氧化矽(SiO2 )等二氧化矽、水鋁石、氫氧化鋁、氫氧化鎂、矽酸鋁、矽酸鎂、滑石、黏土、雲母等。可僅使用該等中之1種，亦可將2種以上組合使用。
無機充填材(C)之平均粒徑無特別限定，宜為0.5~2.0μm，較宜為0.5~1.0μm。無機充填材(C)之平均粒徑若在上述範圍內，即可做成成型性良好的無機充填材(C)。無機充填材(C)之平均粒徑意指利用雷射繞射散射法求得之粒度分布中累積值50%的粒徑。
相對於熱硬化性樹脂(A)100質量份，無機充填材(C)含量宜為150質量份以下，較宜為100質量份以下。
又，樹脂組成物亦可不含無機充填材(C)。樹脂組成物若不含無機充填材(C)，比起樹脂組成物含有無機充填材(C)之情況，更能減少因溫度變化所致半導體封裝件之翹曲量。此外，更可減少除膠渣蝕刻量，從而提升印刷配線板之導通可靠性。 (硬化劑)
樹脂組成物更可含有硬化劑。硬化劑譬如可使用二氰二胺、辛酸鋅等。 (硬化促進劑)
樹脂組成物更可含有硬化促進劑。硬化促進劑譬如可使用咪唑化合物、胺系化合物、硫醇化合物、金屬皂等有機酸金屬鹽等。 (添加劑)
樹脂組成物更可含有添加劑。添加劑譬如可使用熱可塑性樹脂、阻燃劑、著色劑、耦合劑等。 [樹脂組成物之調製方法]
樹脂組成物之調製方法可舉如將熱硬化性樹脂(A)、橡膠成分(B)及其他應需求摻合之成分準備各自預定的摻合量，使該等在有機溶劑中摻合並進一步攪拌、混合之方法等。要於樹脂組成物中摻合無機充填材(C)時，亦可將無機充填材(C)以外之成分摻合於有機溶劑中，獲得清漆狀之基底樹脂後，再於所得基底樹脂摻合無機充填材(C)。有機溶劑譬如可使用醚類、丙酮、甲基乙基酮(MEK)、二甲基甲醯胺、苯、甲苯等。醚類可使用乙二醇單甲基醚等。 [強化纖維基材]
預浸體具備強化纖維基材。強化纖維譬如可使用玻璃纖維、芳香族聚醯胺、液晶聚酯、聚(對伸苯基苯并二㗁唑)(PBO)、聚伸苯硫樹脂(PPS)等，其中又宜使用玻璃纖維。
玻璃纖維譬如可使用E玻璃纖維、D玻璃纖維、S玻璃纖維、T玻璃纖維、NE玻璃纖維、石英纖維(Q玻璃)等。其中，玻璃纖維又宜使用選自E玻璃纖維、T玻璃纖維、S玻璃纖維、NE玻璃纖維及石英纖維(Q玻璃)中之至少1種。藉此，可做成電絕緣性、介電特性更為優異的預浸體之硬化物。
強化纖維之表面可業經耦合劑改質。耦合劑譬如可使用γ-環氧丙氧基丙基三甲氧矽烷、γ-胺丙基三乙氧矽烷、N-苯基-γ-胺丙基三甲氧矽烷等。
強化纖維基材之形態可舉如平織等縱線及橫線幾乎正交編織而成的織布；不織布等。強化纖維基材之厚度宜為10~100μm。 [預浸體製造方法]
預浸體之製造方法可舉如使上述樹脂組成物浸潤至強化纖維基材而獲得浸潤樹脂之基材後，將所得浸潤樹脂之基材加熱乾燥並除去樹脂組成物中之溶劑，使樹脂組成物半硬化之方法等。加熱乾燥之溫度宜為110~150℃。 [覆金屬積層板]
本實施形態之覆金屬積層板(以下有時稱作覆金屬積層板)具備一片預浸體之硬化物或多片預浸體之積層物的硬化物(以下有時稱做第一絕緣層)及接著在該硬化物之單面或雙面的金屬箔。亦即，覆金屬積層板之構造為2層構造或3層構造。2層構造之覆金屬積層板具備第一絕緣層及接著在該第一絕緣層單面之金屬箔。3層構造之覆金屬積層板具備第一絕緣層及接著在該第一絕緣層雙面之金屬箔。
第一絕緣層係由上述預浸體之硬化物所構成，所以第一絕緣層之材料特性與上述預浸體之硬化物的材料特性相同。換言之，第一絕緣層的玻璃轉移溫度(Tg)為150℃以上且220℃以下。所以，使用本實施形態之覆金屬積層板作為半導體封裝件之材料，可減少因溫度變化所致半導體封裝件之翹曲量。
覆金屬積層板之厚度無特別限定，宜為20~400μm。
金屬箔譬如可使用銅箔、銀箔、鋁箔、不鏽鋼箔等，其中又宜使用銅箔。金屬箔之厚度宜為1~12μm。
覆金屬積層板之製造方法可舉如下列方法：將預浸體數片疊合而獲得積層物，再於所得積層物單側或兩側配置金屬箔而獲得附金屬箔之積層物後，將該附金屬箔之積層物加熱加壓成形予以積層一體化之方法；及，將金屬箔配置於一片預浸體之單面或雙面而獲得附金屬箔之預浸體後，將該附金屬箔之預浸體加熱加壓成形予以積層一體化之方法等。加熱加壓成形之條件譬如為140~200℃、0.5~5.0MPa、40~240分鐘。 [印刷配線板]
本實施形態之印刷配線板(以下稱作印刷配線板)具備一片預浸體之硬化物或多片預浸體之積層物之硬化物(以下有時稱作第二絕緣層)及設置在硬化物之單面或雙面的導體配線。印刷配線板包含單層結構之印刷配線板(以下有時稱作芯基板)及多層結構之印刷配線板等。單層結構之印刷配線板係由第二絕緣層及該第二絕緣層之單面或雙面的導體配線構成。多層結構之印刷配線板係於芯基板之形成有導體配線之面上交錯形成有第二絕緣層(以下有時稱作層間絕緣層)與內層導體配線(以下有時稱做內層導體配線)而構成，且最外層形成有導體配線。多層結構之印刷配線板層數無特別限定。
第二絕緣層係由上述預浸體之硬化物所構成，所以第二絕緣層之材料特性與上述預浸體之硬化物的材料特性相同。換言之，第二絕緣層的玻璃轉移溫度(Tg)為150℃以上且220℃以下。所以，使用本實施形態之印刷配線板作為半導體封裝件之材料，可減少因溫度變化所致半導體封裝件之翹曲量。
單層結構之印刷配線板的製造方法無特別限定，可舉如減成法、半加成法等。減成法係以蝕刻除去上述覆金屬積層板的部分金屬箔而形成導體配線之方法。半加成法係以蝕刻除去上述覆金屬積層板之全部金屬箔而獲得積層體之硬化物後，利用無電鍍鍍覆於所得積層體之硬化物的單面或雙面形成一薄層的無電鍍鍍覆層，且以抗鍍阻劑保護非電路形成部後，利用電鍍於電路形成部厚厚地鍍上一電鍍層，然後除去抗鍍阻劑，再以蝕刻除去電路形成部以外之無電鍍鍍覆層而形成導體配線之方法。多層結構之印刷配線板的製造方法無特別限定，可舉如增層法(build-up process)等。 實施例
以下以實施例具體說明本發明。 [實施例1~56及比較例1~8] [樹脂組成物]
準備了下列項目作為樹脂組成物之原料。將硬化性樹脂(A)、橡膠成分(B)、無機充填材(C)及硬化促進劑以表1~表7所示比率摻合並以溶劑(甲基乙基酮)稀釋後，將之攪拌、混合均勻而調製出樹脂組成物。 ＜(A)成分：熱硬化性樹脂＞
(環氧樹脂) ･品名「EPPN-502H」(三苯甲烷型環氧樹脂、日本化藥股份有限公司製、環氧當量：170g/eq) ･品名「NC-3000」(聯苯芳烷基型環氧樹脂、日本化藥股份有限公司製、環氧當量：275g/eq) ･品名「NC-3500」(聯苯芳烷基型環氧樹脂、日本化藥股份有限公司製、環氧當量：209g/eq) ･品名「HP-9500」(萘型環氧樹脂、DIC股份有限公司製、環氧當量：230g/eq)) ･品名「HP-4710」(萘型環氧樹脂、DIC股份有限公司製、環氧當量170g/eq) ･品名「YX7400」(環氧樹脂、三菱化學股份有限公司製、環氧當量：440g/eq) 環氧當量為目錄值。 (酚樹脂) ･品名「TD-2090」(酚醛型酚樹脂、DIC股份有限公司製、羥基當量：105g/eq) ･品名「MEH-7600」(四酚型酚樹脂、明和化成股份有限公司、羥基當量：100g/eq) ･品名「GPH-103」(聯苯芳烷基型酚樹脂、日本化藥股份有限公司、羥基當量：230g/eq) ･品名「HPC-9500」(萘型酚樹脂、DIC股份有限公司製、羥基當量：153g/eq) ･品名「TD-2093Y」(酚醛型酚樹脂、DIC股份有限公司製、羥基當量：104g/eq) ･品名「HPC-9100」(磷改質酚樹脂、DIC股份有限公司製、羥基當量：373g/eq) 羥基當量為目錄值。 (雙馬來亞醯胺樹脂) ･品名「MIR-3000」(馬來亞醯胺、日本化藥股份有限公司製) ･品名「BMI-2300」(苯甲烷馬來亞醯胺、大和化成工業股份有限公司製) (氰酸酯樹脂) ･品名「BADCy」(雙酚A型氰酸酯樹脂、Lonza Japan股份有限公司製)。 ＜(B)成分：重量平均分子量為10萬以上之高分子成分及/或內核外殼橡膠＞
(重量平均分子量為10萬以上之高分子成分(B2)) ･品名「SG-P3改197」(丙烯酸樹脂、Nagase ChemteX Co., Ltd.製) 該丙烯酸樹脂(品名「SG-P3改197」)的環氧值為0.17ep/kg，重量平均分子量為70萬。 ･品名「SG-P3Mw1」(丙烯酸樹脂、Nagase ChemteX Co., Ltd.製) 該丙烯酸樹脂(品名「SG-P3Mw1」)係分子中具有上述式(1)及(2)所示重複單元(式(1)之R1為氫原子，式(2)之R2為丁基、乙基)，具有環氧基且於碳原子間不具不飽和鍵之樹脂。該丙烯酸樹脂(品名「SG-P3Mw1」)的環氧值為0.21ep/kg，重量平均分子量為26萬。 ･品名「SG-80H」(丙烯酸樹脂、Nagase ChemteX Co., Ltd.製) 該丙烯酸樹脂(品名「SG-80H」)的環氧值為0.07ep/kg，重量平均分子量為35萬。 (內核外殼橡膠(B1))
･品名「SRK200A」(內核外殼型多層結構橡膠、內核相：聚矽氧/丙烯酸聚合物、外殼相：丙烯腈/苯乙烯、平均粒徑：0.15μm、Mitsubishi Rayon Co., Ltd.製) ･品名「S-2100」(內核外殼型多層結構橡膠、內核相：聚矽氧/丙烯酸聚合物、外殼相：聚甲基丙烯酸甲酯、平均粒徑：0.70μm、Mitsubishi Rayon Co., Ltd.製) ･品名「SX-005」(內核外殼型多層結構橡膠、內核相：聚矽氧/丙烯酸聚合物、外殼相：聚甲基丙烯酸甲酯、平均粒徑：0.20μm、Mitsubishi Rayon Co., Ltd.製) ･品名「AC3816」(內核外殼型多層結構橡膠、內核相：交聯丙烯酸聚合物、外殼相：聚甲基丙烯酸甲酯、平均粒徑：0.3μm、Aica Kogyo Co., Ltd.製) ･品名「MX-217」(內核外殼橡膠、KANEKA股份有限公司製)。 ＜(C)成分：無機充填材＞
･品名「SC-2500SEJ」(熔融二氧化矽粒子、平均粒徑：0.5μm、Admatechs Co., Ltd.製)。 ＜硬化促進劑＞
･品名「2E4MZ」(咪唑、四國化成工業股份有限公司製) ･品名「Zn-OCTOATE」(辛酸鋅、DIC股份有限公司製)。 (預浸體) 將玻璃布(日東紡績股份有限公司製♯2118型、WTX2118T-107-S199、T玻璃)浸泡至樹脂組成物中以使預浸體之硬化物厚度成為100μm。以非接觸型加熱組件將浸潤至玻璃布中的樹脂組成物加熱乾燥直到成為半硬化狀態為止。加熱溫度為150~160℃。藉此除去樹脂組成物中之溶劑，而製造出具備玻璃布及浸潤至該玻璃布中之樹脂組成物之半硬化物的預浸體。相對於預浸體100質量份，預浸體之樹脂含量(樹脂量)為41質量份。 (覆金屬積層板) 將兩片預浸體疊合而獲得一積層物，再於所得積層物兩面疊合作為金屬箔之銅箔(厚：12μm)而獲得附銅箔之積層物。將該附銅箔之積層物加熱加壓成形，製造出厚0.2mm之雙面覆金屬積層板。加熱加壓成形之條件為210℃、4MPa、120分鐘。 [測定材料特性及評估翹曲特性]
上述玻璃布係由縱線及橫線幾乎正交編織而成的織布所構成。以蝕刻除去接著在雙面覆金屬積層板兩面的銅箔，獲得一積層物之硬化物。在該積層物之硬化物對玻璃布之縱線或橫線斜45°角的方向(斜向方向)將該積層物之硬化物裁切，製作出尺寸為50mm×5mm之試料。使用該試料，利用下述方法測定Tg(DMA･拉伸)及彈性係數(260℃･DMA･拉伸･斜向)。並進一步評估除膠渣耐性及擺幅量(30-260℃)。材料特性之測定結果以及除膠渣耐性及擺幅量的評估結果列於表1~表7。 ＜Tg(DMA･拉伸)＞
針對上述試料，以動態黏彈性測定裝置(SII NanoTechnology Inc.製「DMS6100」)在5℃/分鐘之升溫條件(DMA法)下測定tanδ，並以其尖峰溫度作為玻璃轉移溫度(Tg)。 ＜彈性係數(260℃･DMA･拉伸･斜向)＞
利用DMA測定在260℃之氣體環境下測定上述試料之彈性係數(動態儲存彈性模數)。 ＜除膠渣耐性＞
除膠渣耐性係從下述試驗片進行除膠渣處理前之處理前試驗片的質量與下述試驗片經過錳酸鹽行除膠渣處理後之處理完畢之試驗片的質量之差，計算除膠渣蝕刻量，並依其計算值來作評估。
具體上，係以蝕刻除去接著在尺寸10cm×10cm之雙面覆金屬積層板的銅箔而獲得試驗片。並從所得試驗片進行除膠渣處理前之處理前試驗片的質量(初始質量)，與所得試驗片以下列條件行除膠渣處理後之處理完畢之試驗片的質量之差(單位為mg/cm2 )，算出除膠渣蝕刻量。
處理前試驗片之初始質量測定係使試驗片在100℃下乾燥1小時且在150℃下乾燥1小時後，在乾燥器內空冷1日後再進行。
處理完畢之試驗片的質量測定係如下進行。首先，將測定初始質量後之處理前試驗片以Rohm and Haas Co.製「MLB211」及「CupZ」膨潤5分鐘後，再以Rohm and Haas Co.製「MLB213A-1」及「MLB213B-1」進行6分鐘微浸蝕處理。接著，以Rohm and Haas Co.製「MLB216-2」中和5分鐘，在130℃下乾燥30分鐘後，在乾燥器內空冷1天後再測定處理完畢之試驗片的質量。
除膠渣蝕刻量為1.0mg/cm2 以下時，評估為除膠渣耐性優異。 ＜擺幅量(30-260℃)＞
以減成法蝕刻除去接著在雙面覆金屬積層板兩面的部分銅箔後，形成導體配線而製造出印刷配線板。將半導體晶片(尺寸：10mm×10mm×厚0.10mmt)以倒裝晶片方式安裝於印刷配線板上並進行迴焊處理(260℃)。然後，將半導體晶片與印刷配線板之間以底部填膠材(Panasonic Co.製「CV5300」)充填，將半導體晶片接著固定於印刷配線板上而製造出半導體封裝件(12.5mm×12.5mm×厚0.27mmt)。
接著，以搭載有半導體晶片之面向下側的方式將半導體封裝件配置於翹曲測定裝置(AKROMETRIX公司製「THERMOIRE PS200」)內，根據陰影疊紋(Shadow Moire)測定理論測出3維形狀並依其所得來測定半導體封裝件在30~260℃下的翹曲量。表1中，符號「+」表示半導體封裝件向上反凸之狀態(呈微笑形狀)。符號「-」表示半導體封裝件向下反凸之狀態(呈哭喪形狀)。
半導體封裝件之擺幅量係根據上述翹曲量之測定值，以符號(+)及(-)之位移量計。具體上係將半導體封裝件從30℃加熱至260℃，然後再冷卻至30℃時取翹曲量之最大值與最小值之差，求出半導體封裝件之擺幅量。該擺幅量愈小，愈具有低翹曲特性。
擺幅量(30-260℃)為100μm以下時，評估為可減少因溫度變化所致半導體封裝件之翹曲量。
[表1]
[表2]
[表3]
[表4]
[表5]
[表6]
[表7]

Claims (6)

  1. 一種預浸體，其特徵在於具備強化纖維基材及浸潤在前述強化纖維基材中之樹脂組成物的半硬化物，且硬化後玻璃轉移溫度(Tg)為150℃以上且220℃以下；前述樹脂組成物含有：(A)熱硬化性樹脂；及(B)內核外殼橡膠與重量平均分子量10萬以上之高分子成分二者，或者僅內核外殼橡膠；相對於前述(A)成分100質量份，前述(B)成分之含量為30質量份以上且100質量份以下。
  2. 如請求項1之預浸體，其中前述樹脂組成物更含有(C)無機充填材。
  3. 如請求項2之預浸體，其中相對於前述(A)成分100質量份，前述(C)成分之含量為150質量份以下。
  4. 如請求項1至3中任一項之預浸體，其中前述(A)成分係由選自於由環氧樹脂、酚樹脂、雙馬來亞醯胺樹脂及氰酸酯樹脂所構成群組中之至少1種所構成。
  5. 一種覆金屬積層板，其特徵在於具備一片如請求項1至4中任一項之預浸體的硬化物或多片該預浸體之積層物的硬化物，及接著在前述硬化物之單面或雙面的金屬箔。
  6. 一種印刷配線板，其特徵在於具備一片如請求項1至4中任一項之預浸體的硬化物或多片該預浸體 之積層物的硬化物，及設置在前述硬化物之單面或雙面的導體配線。
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WO2017183621A1 (ja) 2017-10-26
TW201739019A (zh) 2017-11-01

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