CN109071854B - 预浸料、覆金属层压板和印刷线路板 - Google Patents

预浸料、覆金属层压板和印刷线路板 Download PDF

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CN109071854B
CN109071854B CN201780024355.6A CN201780024355A CN109071854B CN 109071854 B CN109071854 B CN 109071854B CN 201780024355 A CN201780024355 A CN 201780024355A CN 109071854 B CN109071854 B CN 109071854B
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prepreg
component
resin
cured product
mass
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CN109071854A (zh
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小畑心平
高桥龙史
星野泰范
藤田茂利
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Panasonic Intellectual Property Management Co Ltd
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Panasonic Intellectual Property Management Co Ltd
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    • 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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Abstract

提供了预浸料，其具有增强纤维基材和浸渍该增强纤维基材的树脂组合物的半固化产物。固化后，预浸料可以具有含端点的150℃至220℃的玻璃化转变温度(Tg)。树脂组合物含有(A)热固性树脂和(B)至少一种选自由核壳型橡胶和重均分子量为100000以上的聚合物组分组成的组中的化合物。相对于100质量份的(A)组分，(B)组分的含量为含端点的30至100质量份。

Description

预浸料、覆金属层压板和印刷线路板
技术领域
本发明涉及预浸料、覆金属层压板和印刷线路板。
背景技术
印刷线路板广泛用于多个技术领域，如电子设备、通信设备和计算器。近年来，特别小的移动设备如移动通信设备和笔记本电脑已经快速地变得越来越多样化、高性能、薄和小。因此，在这样的设备中使用的印刷线路板需要具有更小的导体线路、具有多层导电线路层、更薄、并且能够具有更高的性能以及高机械特性。尤其是，由于印刷线路板变得越来越薄，出现了在包括安装在印刷线路板上的半导体芯片的半导体封装中发生翘曲的问题。这样的具有翘曲的半导体封装可能不能适当地结合到电子设备中。
为了防止包括安装在印刷线路板上的半导体芯片的半导体封装的翘曲，专利文献1公开了一种覆金属层压板，其包括在绝缘层的两个表面上的金属箔，所述绝缘层包含环氧树脂组合物和纤维基材，其中所述环氧树脂组合物含有环氧树脂、双马来酰亚胺化合物和无机填料，并且在30至260℃温度范围内的覆金属层压板的尺寸变化的滞后处于一定范围内。公开了由于环氧树脂组合物含有双马来酰亚胺化合物，并且所述滞后处于一定范围内，即使发生大的温度变化，如超过绝缘层的玻璃化转变温度的温度，在30至260℃范围内在绝缘层的平面方向(XY方向)上计算的平均线性膨胀系数小，并且可以减少其中半导体元件安装在印刷线路板上的半导体设备在室温(23℃)和在260℃的翘曲。
然而，存在专利文献1中所公开的覆金属层压板不能充分防止半导体封装的翘曲的问题。
另外，对印刷线路板进行钻孔和激光加工以形成用于连接在多层上形成的导体图案的孔。当孔形成时，倾向于在孔的内壁上产生树脂污迹(smear)。由于此原因，需要除污迹(desmear)过程来去除树脂污迹。通过使用例如高锰酸盐如高锰酸钾来进行除污迹过程。
然而，当通过除污迹过程去除的树脂污迹的量(除污迹刻蚀的量)大时，发生孔的形变和铜箔的剥离，导致印刷线路板的传导可靠性降低。因此，需要减少除污迹刻蚀的量，即改善除污迹耐性。
引用清单
专利文献
专利文献1：JP 2015-63040 A
发明概述
本发明的目的是提供预浸料、覆金属层压板和印刷线路板，其中即使在印刷线路板薄时，也可以减少由于温度变化造成的半导体封装的翘曲，并且除污迹耐性也是出色的。
根据本发明的一个实施方案的预浸料包含：含有增强纤维的基材；和浸渍到含有增强纤维的基材中的树脂组合物的半固化产物，其中固化后的预浸料的玻璃化转变温度(Tg)高于或等于150℃且低于或等于220℃，所述树脂组合物含有：(A)热固性树脂；和(B)至少一种选自由核壳型橡胶和重均分子量为100000以上的聚合物组分组成的组中的化合物，并且相对于100质量份的(A)组分，(B)组分的量高于或等于30质量份且低于或等于100质量份。
根据本发明的一个实施方案的覆金属层压板含有：一片预浸料的或两片以上预浸料的堆叠体的固化产物；和结合到固化产物的一面或两面的金属箔。
根据本发明的一个实施方案的印刷线路板含有：一片预浸料的或两片以上预浸料的堆叠体的固化产物；和设置在固化产物的一面或两面上的导体线路。
实施方案描述
在下文中，说明本发明的一个实施方案。
[预浸料]
根据本实施方案的预浸料(在下文中也称为预浸料)包含：含有增强纤维的基材；和浸渍到含有增强纤维的基材中的树脂组合物的半固化产物，其中固化后的预浸料的玻璃化转变温度(Tg)高于或等于150℃且低于或等于220℃。树脂组合物含有(A)热固性树脂；和(B)至少一种选自由核壳型橡胶(在下文中也称为核壳型橡胶(B1))和重均分子量为100000以上的聚合物组分(在下文中也称为聚合物组分(B2))组成的组中的化合物(在下文中也称为橡胶组分(B))。相对于100质量份的(A)组分，橡胶组分(B)((B)组分)的量高于或等于30质量份且低于或等于100质量份。当使用本实施方案的预浸料作为用于包括安装在印刷线路板上的半导体芯片的半导体封装的材料时，在不调整树脂组成以使得预浸料的固化产物在260℃的弹性模量变高并且预浸料的固化产物的热膨胀系数在一定范围内的情况下，可以有效地降低半导体芯片和印刷电路板中的应力，并且可以减少由于温度变化造成的半导体封装的翘曲。另外，当将本实施方案的预浸料用于印刷线路板时，在形成用于连接层的孔时产生的树脂污迹的除污迹刻蚀的量变少，由此印刷线路板的传导可靠性不太可能降低。
预浸料的固化产物的玻璃化转变温度(Tg)高于或等于150℃且低于或等于220℃，优选高于或等于160℃且低于或等于200℃，更优选高于或等于180℃且低于或等于200℃。当预浸料的固化产物的玻璃化转变温度(Tg)高于220℃时，由于温度变化造成的半导体封装的翘曲可能增大。另外，当预浸料的固化产物的玻璃化转变温度(Tg)低于150℃时，除污迹耐性可能不充足。
预浸料的固化产物在260℃的弹性模量优选高于或等于0.5GPa且低于或等于7.0GPa，并且更优选高于或等于0.5GPa且低于或等于5.0GPa。当预浸料的固化产物在260℃的弹性模量在上述范围内时，可以更大程度地减少由于温度变化造成的半导体封装的翘曲。
预浸料的厚度可以通过使用两侧覆金属层压板根据所需性质适当地选择，并且优选在0.010至0.200mm的范围内。相对于100质量份的预浸料，预浸料的树脂含量(树脂组合物的量)优选在30至80质量份的范围内。
[树脂组合物的半固化产物]
通过使树脂组合物半固化来形成树脂组合物的半固化产物。
树脂组合物含有热固性树脂(A)和橡胶组分(B)，并且如果需要的话，还含有无机填料(C)、固化剂、固化促进剂和添加剂。
{热固性树脂(A)}
树脂组合物含有热固性树脂(A)。例如，可以使用环氧树脂、酚醛树脂、双马来酰亚胺树脂和氰酸酯树脂作为热固性树脂(A)。可以单独使用以上列出的化合物中的一种，并且可以组合使用以上列出的化合物中的两种以上，作为热固性树脂(A)。热固性树脂(A)优选地含有至少一种选自由以下各项组成的组中的化合物(在下文中称为热固性树脂(A1))：环氧树脂、酚醛树脂、双马来酰亚胺树脂和氰酸酯树脂。
(环氧树脂)
环氧树脂的实例可以包括双酚环氧树脂、酚醛清漆环氧树脂、联苯基环氧树脂、二甲苯环氧树脂、芳基亚烷基环氧树脂、萘环氧树脂、萘骨架改性的环氧树脂、三苯基甲烷环氧树脂、蒽环氧树脂、二环戊二烯环氧树脂、降冰片烯环氧树脂、芴环氧树脂和通过将之前列出的环氧树脂卤化获得的阻燃性环氧树脂。可以单独使用以上列出的化合物中的一种，并且可以组合使用以上列出的化合物中的两种以上。双酚环氧树脂的实例可以包括双酚A环氧树脂、双酚F环氧树脂、双酚S环氧树脂。酚醛清漆环氧树脂的实例可以包括苯酚酚醛清漆环氧树脂和甲酚酚醛清漆环氧树脂。芳基亚烷基环氧树脂的实例可以包括苯酚芳烷基环氧树脂、联苯基芳烷基环氧树脂、联苯基酚醛清漆环氧树脂、联苯基二亚甲基环氧树脂、三苯酚甲烷酚醛清漆环氧树脂和四甲基联苯基环氧树脂。萘骨架改性的环氧树脂的实例可以包括萘骨架改性的甲酚酚醛清漆环氧树脂、萘二酚芳烷基环氧树脂、萘酚芳烷基环氧树脂、甲氧基萘改性的甲酚酚醛清漆环氧树脂和甲氧基萘二亚甲基环氧树脂。
环氧树脂的环氧基当量优选大于或等于180g/eq，并且更优选大于或等于200g/eq。当环氧基当量大于或等于180g/eq时，树脂组合物的固化产物的交联密度不太可能高，并且预浸料的固化产物的玻璃化转变温度不太可能超过220℃。注意，环氧基当量是平均分子量除以一个分子中的环氧基的数量。羟基当量是平均分子量除以一个分子中的羟基的数量。
(酚醛树脂)
酚醛树脂的实例可以包括联苯基芳烷基酚醛树脂、苯基芳烷基酚醛树脂、酚醛清漆酚醛树脂、甲酚酚醛清漆酚醛树脂、双酚A酚醛清漆酚醛树脂、萘酚醛树脂、四苯酚酚醛树脂和磷改性的酚醛树脂。可以单独使用以上列出的化合物中的一种，并且可以组合使用以上列出的化合物中的两种以上。
酚醛树脂的羟基当量优选大于或等于140g/eq，并且更优选大于或等于200g/eq。当羟基当量大于或等于140g/eq时，树脂组合物的固化产物的交联密度不太可能高，并且预浸料的固化产物的玻璃化转变温度不太可能高。
(双马来酰亚胺树脂)
双马来酰亚胺树脂的实例可以包括4，4’-二苯基甲烷双马来酰亚胺、苯基甲烷马来酰亚胺、间亚苯基双马来酰亚胺、双酚A二苯基醚双马来酰亚胺、3，3’-二甲基-5，5’-二乙基-4，4’-二苯基甲烷双马来酰亚胺、4-甲基-1，3-亚苯基双马来酰亚胺和1，6’-双马来酰亚胺-(2，2，4-三甲基)己烷。可以单独使用以上列出的化合物中的一种，并且可以组合使用以上列出的化合物中的两种以上。
(氰酸酯树脂)
每分子具有两个以上氰酸酯基的化合物作为氰酸酯树脂是优选的，并且氰酸酯树脂的实例可以包括2，2-双(4-氰酸苯基)丙烷(双酚A氰酸酯树脂)、双(3，5-二甲基-4-氰酸苯基)甲烷、2，2-双(4-氰酸苯基)乙烷和芳族氰酸酯化合物如之前列出的化合物的衍生物。可以单独使用以上列出的化合物中的一种，并且可以组合使用以上列出的化合物中的两种以上。
{橡胶组分(B)}
树脂组合物含有至少一种选自由核壳型橡胶(B1)和重均分子量为100000以上的聚合物组分(B2)组成的组中的化合物(B)。换言之，根据其他组分如热固性树脂(A)，树脂组合物可以含有以下各项作为橡胶组分(B)：组合的核壳型橡胶(B1)和聚合物组分(B2)；单独的核壳型橡胶(B1)；或单独的聚合物组分(B2)。考虑到翘曲性质和可加工性(如，例如，激光可加工性)之间的平衡，树脂组合物优选地含有核壳型橡胶(B1)和聚合物组分(B2)两者。
相对于100质量份的(A)组分，橡胶组分(B)的量高于或等于30质量份且低于或等于100质量份。当橡胶组分(B)的量高于100质量份时，如之后说明的，用于形成预浸料的清漆形式的基体树脂的粘度存在升高的可能性，这可能导致差的预浸料形成。当橡胶组分(B)的量低于30质量份时，由于温度变化造成的半导体封装的翘曲可能增加。
当橡胶组分(B)含有核壳型橡胶(B1)和之后说明的丙烯酸树脂(B2a)时，相对于100质量份的(A)组分，核壳型橡胶(B1)和丙烯酸树脂(B2a)的总量优选高于或等于50质量份且低于或等于100质量份，并且更优选高于或等于60质量份且低于或等于80质量份。当核壳型橡胶(B1)和丙烯酸树脂(B2a)的总量在上述范围内时，可以减少由于温度变化造成的半导体封装的翘曲。
(核壳型橡胶(B1))
核壳型橡胶(B1)是具有核壳型结构的橡胶组分，在所述核壳型结构中，中心部分(核)和围绕所述中心的部分(壳)由不同的聚合物制成。
构成核的聚合物的实例可以包括有机硅/丙烯酸聚合物、丙烯酸聚合物、有机硅聚合物、丁二烯聚合物和异戊二烯聚合物。构成壳的聚合物的实例可以包括聚甲基丙烯酸甲酯和聚苯乙烯。
核壳型橡胶(B1)的具体实例可以包括：MITSUBISHI RAYON CO.，LTD.制造的产品名“S2100”、“SX-005”、“S-2001”、“S-2006”、“S-2030”、“S-2200”、“SRK200A”和“SX-006”；Aica Kogyo Co.，Ltd.制造的产品名“AC3816”、“AC3816N”、“AC3832”、“AC4030”、“AC3364”、“IM101；以及KANEKA CORPORATION制造的产品名“MX-217”、“MX-153”和“MX-960”。
(聚合物组分(B2))
聚合物组分(B2)的重均分子量为100000以上，并且在改善成形性方面优选为850000以下。当聚合物组分(B2)的重均分子量小于100000时，半导体芯片和印刷线路板中的应力不能充分降低，并且由于温度变化造成的半导体封装的翘曲可能增加。
作为聚合物组分(B2)，可以使用弹性体如丙烯酸树脂和有机硅树脂。可以单独使用这样的化合物中的一种，并且可以组合使用这样的化合物中的两种以上。优选地使用丙烯酸树脂作为聚合物组分(B2)。当橡胶组分(B)含有丙烯酸树脂时，可以降低预浸料的固化产物的弹性，并且可以更大程度地减少由于温度变化造成的半导体封装的翘曲。
优选地使用具有至少一个选自由以下式(1)、(2)和(3)表示的结构组成的组中的结构的丙烯酸树脂(B2a)作为丙烯酸树脂。
[化学式1]
Figure BDA0001833171440000071
Figure BDA0001833171440000072
Figure BDA0001833171440000073
x表示大于或等于0的整数。y表示大于或等于0的整数。z表示大于或等于0的整数。注意，不包括x、y和z都是0的情况。在式(2)中，R1表示氢原子或甲基，并且R2表示氢原子或烷基。在式(3)中，R3表示氢原子或甲基，并且R4表示选自由-Ph(苯基)、-COOCH2Ph和-COO(CH2)2Ph组成的组中的至少一个基团。
换言之，丙烯酸树脂(B2a)的主链优选地具有由在上述式(1)、(2)和(3)中的至少式(2)和(3)表示的结构。另外，丙烯酸树脂(B2a)可以在其分子内含有环氧基。
当丙烯酸树脂(B2a)的主链具有由式(1)、(2)和(3)中的全部表示的结构时，由式(1)、(2)和(3)表示的各结构的先后顺序没有特别限制。在丙烯酸树脂(B2a)的主链中，两个以上由式(1)表示的结构可以是连续或不连续的，两个以上由式(2)表示的结构可以是连续或不连续的，并且两个以上由式(3)表示的结构可以是连续或不连续的。
当丙烯酸树脂(B2a)的主链具有由式(2)和(3)表示的结构时，由式(2)和(3)表示的各结构的先后顺序没有特别限制。在丙烯酸树脂(B2a)的主链中，两个以上由式(2)表示的结构可以是连续或不连续的，并且两个以上由式(3)表示的结构可以是连续或不连续的。
由式(3)表示的结构可以具有Ph(苯基)、-COOCH2Ph和-COO(CH2)2Ph。丙烯酸树脂(B2a)优选地不含在碳原子之间的不饱和键如双键和三键。换言之，丙烯酸树脂(B2a)中的碳原子优选地通过饱和键(单键)键合。丙烯酸树脂(B2a)的重均分子量(Mw)优选为200000至850000。
(无机填料(C))
树脂组合物还可以含有无机填料(C)。当树脂组合物含有无机填料(C)时，可以减少预浸料的固化产物的热膨胀。
无机填料(C)的实例可以包括二氧化硅如熔融二氧化硅(SiO2)和晶体二氧化硅(SiO2)、水铝石、氢氧化铝、氢氧化镁、硅酸铝、硅酸镁、滑石、粘土和云母。可以单独使用以上列出的化合物中的一种，并且可以组合使用以上列出的化合物中的两种以上。
无机填料(C)的平均粒度没有特别限制，并且优选地在0.5至2.0μm的范围内，并且更优选地在0.5至1.0μm的范围内。当无机填料(C)的平均粒度在0.5至2.0μm的范围内时，树脂组合物的成形性可以是良好的。无机填料(C)的平均粒度是在通过激光衍射/散射法测量的粒度分布中的中值粒度。
相对于100质量份的热固性树脂(A)，无机填料(C)的量优选小于或等于150质量份，并且更优选小于或等于100质量份。
树脂组合物不需要含有无机填料(C)。当树脂组合物不含无机填料(C)时，与树脂组合物含有无机填料(C)的情况相比，可以更大程度地减少由于温度变化造成的半导体封装的翘曲。另外，可以更大程度地减少除污迹刻蚀的量，由此改善印刷线路板的传导可靠性。
(固化剂)
树脂组合物还可以含有固化剂。固化剂的实例可以包括双氰胺和辛酸锌。
(固化促进剂)
树脂组合物还可以含有固化促进剂。固化促进剂的实例可以包括咪唑化合物、胺化合物、硫醇化合物和有机酸的金属盐如金属皂。
(添加剂)
树脂组合物还可以含有添加剂。添加剂的实例可以包括热塑性树脂、阻燃剂、着色剂和偶联剂。
[树脂组合物的制备方法]
树脂组合物的制备方法的一个实例是将预定量的热固性树脂(A)、橡胶组分(B)和如果需要的话其他组分在有机溶剂中混合和搅拌。在将无机填料(C)加入到树脂组合物中的情况下，可以将树脂组合物的除无机填料(C)以外的所有组分加入到有机溶剂中以获得清漆形式的基体树脂，然后可以将无机填料(C)加入到基体树脂中。有机溶剂的实例可以包括醚、丙酮、甲乙酮(MEK)、二甲基甲酰胺、苯和甲苯。醚的实例可以包括乙二醇单***。
[含有增强纤维的基材]
预浸料包含含有增强纤维的基材。增强纤维的实例可以包括玻璃纤维、芳族聚酰胺、液晶聚酯、聚(对亚苯基苯并二
Figure BDA0001833171440000091
唑)(PBO)和聚苯硫醚树脂(PPS)。特别优选地使用玻璃纤维。
玻璃纤维的实例可以包括E玻璃纤维、D玻璃纤维、S玻璃纤维、T玻璃纤维、NE玻璃纤维和石英纤维(Q纤维)。特别优选的是使用选自由E玻璃纤维、T玻璃纤维、S玻璃纤维、NE玻璃纤维和石英纤维(Q纤维)组成的组中的至少一种作为玻璃纤维。在该情况下，预浸料的固化产物可以具有出色的电气绝缘性质和出色的介电性质。
可以用偶联剂涂覆增强纤维的表面。偶联剂的实例可以包括γ-缩水甘油基氧基丙基三甲氧基甲硅烷、γ-氨基丙基三乙氧基甲硅烷和N-苯基-γ-氨基丙基三甲氧基甲硅烷。
增强纤维的基底可以是以下形式：例如，其中经纱和纬纱如在平纹纺织中一样几乎正交地纺织的纺织物；和无纺布。含有增强纤维的基材的厚度优选地在10至100μm的范围内。
[预浸料的制造方法]
预浸料的制造方法的一个实例是通过将树脂组合物浸渍到含有增强纤维的基材中来获得树脂浸渍的基材，然后通过加热和干燥所得树脂浸渍的基材由此去除树脂组合物中的溶剂来使树脂组合物半固化。优选地在110至150℃的范围内的温度进行加热和干燥。
[覆金属层压板]
本实施方案的覆金属层压板(在下文中称为覆金属层压板)包括：一片预浸料的或两片以上预浸料的堆叠体的固化产物(在下文中称为第一绝缘层)；和与固化产物的一面或两面结合的金属箔。换言之，覆金属层压板具有两层结构或三层结构。两层结构的覆金属层压板包括第一绝缘层和与第一绝缘层的一面结合的金属箔。三层结构的覆金属层压板包括第一绝缘层和与第一绝缘层的两面结合的金属箔。
由于第一绝缘层是预浸料的固化产物，第一绝缘层的材料性质与预浸料的固化产物的材料性质相同。换言之，第一绝缘层的玻璃化转变温度(Tg)高于或等于150℃且低于或等于220℃。因此，当使用本实施方案的覆金属层压板作为用于半导体封装的材料时，可以减少由于温度变化造成的半导体封装的翘曲。
覆金属层压板的厚度没有特别限制，并且优选地在20至400μm的范围内。
金属箔的实例可以包括铜箔、银箔、铝箔和不锈钢箔。特别优选地使用铜箔。金属箔的厚度优选地在1至12μm的范围内。
覆金属层压板的制造方法的实例可以包括：其中将多个预浸料堆叠以获得堆叠体，进一步将金属箔堆叠在所得堆叠体的一面或两面上以获得具有金属箔的堆叠体，然后通过加热和加压使具有金属箔的堆叠体的层一体化的方法；和其中将金属箔堆叠在一个预浸料的一面或两面上以获得具有金属箔的预浸料，然后通过加热和加压使具有金属箔的预浸料的层一体化的方法。加热和加压的条件例如是140至200℃，0.5至5.0MPa，40至240分钟。
[印刷线路板]
本实施方案的印刷线路板(在下文中称为印刷线路板)包括：一片预浸料的或两片以上预浸料的堆叠体的固化产物(在下文中也称为第二绝缘层)；和设置在固化产物的一面或两面上的导体线路。印刷线路板包括：具有单层结构的印刷线路板(在下文中也称为核心板)；和具有多层结构的印刷线路板。具有单层结构的印刷线路板包括所述第二绝缘层和设置在第二绝缘层的一面或两面上的导体线路。在具有多层结构的印刷线路板中，将一个或多个第二绝缘层(在下文中称为层间绝缘层)和在层中的导体线路(在下文中称为层间导体线路)交替地堆叠在核心板的设置导体线路的表面上，并且将导体线路设置在最外表面上。具有多层结构的印刷线路板的层数没有特别限制。
由于第二绝缘层是预浸料的固化产物，第二绝缘层的材料性质与预浸料的固化产物的材料性质相同。换言之，第二绝缘层的玻璃化转变温度(Tg)高于或等于150℃且低于或等于220℃。因此，当使用本实施方案的印刷线路板作为用于半导体封装的材料时，可以减少由于温度变化造成的半导体封装的翘曲。
具有单层结构的印刷线路板的制造方法没有特别限制。具有单层结构的印刷线路板的制造方法的实例可以包括减成法和半加成法。在减成法中，通过去除覆金属层压板的金属箔的一部分来形成导体线路。在半加成法中，通过刻蚀去除覆金属层压板的所有金属箔来获得堆叠体的固化产物，通过化学镀在堆叠体的固化产物的一面或两面上形成薄化学镀层，在未形成电路的表面上形成抗镀剂用于保护，在形成电路的表面上形成厚的一个或多个电镀层，去除抗镀剂，然后通过进行刻蚀去除在未形成电路的表面上的化学镀层来形成导体线路。具有多层结构的印刷线路板的制造方法没有特别限制，并且例如，可以采用累加(buildup)法。
实施例
在下文中，根据实施例具体说明本发明的实施方案。
[实施例1至56以及比较例1至8]
[树脂组合物]
制备以下化合物作为树脂组合物的成分。将热固性树脂(A)、橡胶组分(B)、无机填料(C)和固化促进剂以表1至7中所示的量合并，并且用溶剂(甲乙酮)稀释，将其搅拌和混合用于均匀化，由此获得树脂组合物。
<(A)组分：热固性树脂>
(环氧树脂)
*产品名“EPPN-502H”(三苯基己烷环氧树脂，由Nippon Kayaku Co.，Ltd.制造，环氧基当量：170g/eq)
*产品名“NC-3000”(联苯基芳烷基环氧树脂，由Nippon Kayaku Co.，Ltd.制造，环氧基当量：275g/eq)
*产品名“NC-3500”(联苯基芳烷基环氧树脂，由Nippon Kayaku Co.，Ltd.制造，环氧基当量：209g/eq)
*产品名“HP-9500”(萘环氧树脂，由DIC CORPORATION制造，环氧基当量：230g/eq)
*产品名“HP-4710”(萘环氧树脂，由DIC CORPORATION制造，环氧基当量：170g/eq)
*产品名“YX-7400”(环氧树脂，由Mitsubishi Chemical Corporation制造，环氧基当量：440g/eq)
环氧基当量是在目录中得到的值。
(酚醛树脂)
*产品名“TD-2090”(酚醛清漆酚醛树脂，由DIC CORPORATION制造，羟基当量：105g/eq)
*产品名“MEH-7600”(四苯酚酚醛树脂，由MEIWA PLASTIC INDUSTRIES.LTD.制造，羟基当量：100g/eq)
*产品名“GPH-103”(联苯基芳烷基酚醛树脂，由Nippon Kayaku Co.，Ltd.制造，羟基当量：230g/eq)
*产品名“HPC-9500”(萘酚醛树脂，由DIC CORPORATION制造，羟基当量：153g/eq)
*产品名“TD-2093Y”(酚醛清漆酚醛树脂，由DIC CORPORATION制造，羟基当量：104g/eq)
*产品名“HPC-9100”(磷改性的酚醛树脂，由DIC CORPORATION制造，羟基当量：373g/eq)
羟基当量是在目录中得到的值。
(双马来酰亚胺树脂)
*产品名“MIR-3000”(马来酰亚胺，由Nippon Kayaku Co.，Ltd.制造)
*产品名“BMI-2300”(苯基甲烷马来酰亚胺，由Daiwa Kasei Industry Co.，Ltd.制造)
(氰酸酯树脂)
*产品名“BADCy”(双酚A氰酸酯树脂，由LONZA Japan制造)
<(B)组分：重均分子量为100000以上的聚合物组分和/或核壳型橡胶>
(重均分子量为100000以上的聚合物组分(B2))
*产品名“SG-P3revised197”(丙烯酸树脂，由Nagase ChemteX Corporation制造)
该丙烯酸树脂(产品名“SG-P3revised197”)具有0.17ep/kg的环氧基值和700000的平均分子量。
*产品名“SG-P3Mw1”(丙烯酸树脂，由Nagase ChemteX Corporation制造)
该丙烯酸树脂(产品名“SG-P3 Mw1”)具有由以上式(1)和(2)(式1中的R1表示氢原子，式(2)中的R2是丁基或乙基)表示的重复单元和环氧基，并且没有任何在碳原子之间的不饱和键。该丙烯酸树脂具有0.21ep/kg的环氧基值和260000的平均分子量。
*产品名“SG-80H”(丙烯酸树脂，由Nagase ChemteX Corporation制造)
该丙烯酸树脂(产品名“SG-80H”)具有0.07ep/kg的环氧基值和350000的平均分子量。
(核壳型橡胶(B1))
*产品名“SRK200A”(核壳型多层结构橡胶，核：有机硅/丙烯酸聚合物，壳：丙烯腈/苯乙烯，平均粒度：0.15μm，由MITSUBISHI RAYON CO.，LTD.制造)
*产品名“S-2100”(核壳型多层结构橡胶，核：有机硅/丙烯酸聚合物，壳：聚甲基丙烯酸甲酯，平均粒度：0.70μm，由MITSUBISHI RAYON CO.，LTD.制造)
*产品名“SX-005”(核壳型多层结构橡胶，核：有机硅/丙烯酸聚合物，壳：聚甲基丙烯酸甲酯，平均粒度：0.20μm，由MITSUBISHI RAYON CO.，LTD.制造)
*产品名“AC3816”(核壳型多层结构橡胶，核：交联的丙烯酸聚合物，壳：聚甲基丙烯酸甲酯，平均粒度：0.3μm，由Aica Kogyo Co.，Ltd.制造)
*产品名“MX-217”(核壳型橡胶，由KANEKA CORPORATION制造)
<(C)组分：无机填料>
*产品名“SC-2500SEJ”(熔融二氧化硅颗粒，平均粒度：0.5μm，由AdmatechsCompany Limited制造)
<固化促进剂>
*产品名“2E4MZ”(咪唑，由SHIKOKU CHEMICALS CORPORATION制造)
*产品名“Zn-OCTOATE”(辛酸锌，由DIC CORPORATION制造)
(预浸料)
将树脂组合物浸渍到玻璃布(由Nitto Boseki Co.，Ltd.制造的#2118型，WTX2118T-107-S199，T玻璃)中，以使得预浸料的固化产物具有100μm的厚度。然后使用非接触型加热单元将浸渍到玻璃布中的树脂组合物加热和干燥直到半固化。在150至160℃的温度进行加热。因此，去除树脂组合物中的溶剂，并且获得包括玻璃布和浸渍到玻璃布中的树脂组合物的半固化产物的预浸料。相对于100质量份，预浸料的树脂含量(树脂的量)为41质量份。
(覆金属层压板)
制备两片预浸料的堆叠体，并且将铜箔(厚度：12μm)堆叠在堆叠体的两面上作为金属箔。对所得具有铜箔的堆叠体进行加热和加压以获得厚度为0.2mm的两侧覆金属层压板。加热和加压的条件为210℃，4MPa，和120分钟。
[材料性质的测量和翘曲性质的评价]
上述玻璃布是其中经纱和纬纱几乎正交地纺织的纺织布。去除结合到两侧覆金属层压板的两面的铜箔，并且获得堆叠体的固化产物。将堆叠体的固化产物在朝玻璃布的经纱或纬纱的45°的方向(斜线(bias)方向)上切割，由此获得尺寸为50mm×5mm的样品。用以下方法测量所得样品的Tg(DMA，拉伸)和弹性模量(260℃，DMA，拉伸，斜线)。另外，除污迹耐性和摆幅(swing)量(30至260℃)的评价。测量性质的测量以及除污迹耐性和摆幅量的评价的结果在以下表1至7中示出。
<Tg(DMA，拉伸)>
使用动态力学分析装置(由SII Nano Technology Inc.制造的“DMS6100”)，测量在5℃/min的加热条件(DMA法)下的tanδ，并且将峰温度定义为玻璃化转变温度(Tg)。
<弹性模量(260℃，DMA，拉伸，斜线)>
在大气下在260℃通过DMA测量来测量样品的弹性模量(动态弹性储能模量)。
<除污迹耐性>
通过从在除污迹过程前的样品件的重量中减去在使用高锰酸盐的除污迹过程后通过以下方法制备的样品件的重量来计算除污迹刻蚀的量。
具体地，通过去除与尺寸为10cm×10cm的覆金属层压板的两侧结合的铜箔来获得样品件。通过从在除污迹过程前的样品件的重量(初始重量)中减去在以下条件下的除污迹过程后的样品件的重量来计算除污迹刻蚀的量(单位为mg/cm2)。
在将样品件在100℃干燥1小时，然后在150℃干燥1小时，随后在干燥器中空气冷却一天后测量在除污迹过程前的样品件的初始重量。
用以下方法测量在除污迹过程后的样品件的重量。首先，将在测量其初始重量后的样品件使用由Rohm and Haas制造的“MLB211”和“CupZ”溶胀5分钟，然后使用由Rohm andHaas制造的“MLB213A-1”和“MLB213B-1”进行微刻蚀6分钟。之后，将样品件用由Rohm andHaas制造的“MLB216-2”中和5分钟，在130℃干燥30分钟，并且在干燥器中空气冷却1天。然后，测量重量。
评价等于或小于1.0mg/cm2的除污迹刻蚀的量显示出出色的除污迹耐性。
<摆幅量(30至260℃)>
通过减成法刻蚀与覆金属层压板的两侧结合的铜箔的部分以形成导体线路，由此获得印刷线路板。通过倒装芯片安装将半导体芯片(尺寸：10mm×10mm×厚度0.10mmt)安装在印刷线路板上，并且进行回流过程(260℃)。之后，用底充胶(underfill)(由PanasonicCorporation制造的“CV5300”)填充半导体芯片和印刷线路板之间的空间，以使得半导体芯片牢固地与印刷线路板结合，由此获得半导体封装(12.5mm×12.5mm×厚度0.27mmt)。
然后，将半导体封装放置在翘曲测量装置(由AKROMETRIX制造的“THERMOIREPS200”)中，以使得半导体芯片安装在其上的半导体封装的表面朝下，并且基于ShadowMoiré原理通过3维形状测量来测量半导体封装在30至260℃的翘曲。在表1中，摆幅量的正值意指半导体封装翘曲为使得半导体封装朝上突出(正翘曲形状)。摆幅量的负值意指半导体封装翘曲为使得半导体封装朝下突出(负翘曲形状)。
基于上述翘曲测量，半导体封装的摆幅量为正差或负差。具体地，当将半导体封装从30℃加热到260℃然后冷却到30℃时的翘曲的最大值和最小值之间的差计算为半导体封装的摆幅量。摆幅量越小，半导体封装的翘曲性质越低。
当摆幅量(30至260℃)低于或等于100μm时，评价为减少了由于温度变化造成的半导体封装的翘曲。
[表1]
Figure BDA0001833171440000171
[表2]
Figure BDA0001833171440000181
[表3]
Figure BDA0001833171440000191
[表4]
Figure BDA0001833171440000201
[表5]
Figure BDA0001833171440000211
[表6]
Figure BDA0001833171440000221
[表7]
Figure BDA0001833171440000231

Claims (6)

1.一种预浸料，所述预浸料包含：
含有增强纤维的基材；和
浸渍到所述含有增强纤维的基材中的树脂组合物的半固化产物，
固化后的所述预浸料的玻璃化转变温度(Tg)高于或等于150℃且低于或等于220℃，
所述树脂组合物含有：
(A)组分，其是热固性树脂；和
(B)组分，其是：
重均分子量为100000以上的聚合物组分，或者
由所述聚合物组分和核壳型橡胶构成的组分，
相对于100质量份的(A)组分，(B)组分的量高于或等于30质量份且低于或等于100质量份。
2.根据权利要求1所述的预浸料，所述预浸料还包含(C)组分，其是无机填料。
3.根据权利要求2所述的预浸料，其中
相对于100质量份的(A)组分，(C)组分的量小于或等于150质量份。
4.根据权利要求1所述的预浸料，其中
(A)组分含有至少一种选自由环氧树脂、酚醛树脂、双马来酰亚胺树脂和氰酸酯树脂组成的组中的化合物。
5.一种覆金属层压板，所述覆金属层压板包含：
一片根据权利要求1至4中任一项所述的预浸料的或两片以上根据权利要求1至4中任一项所述的预浸料的堆叠体的固化产物；和
结合到所述固化产物的一个或两个表面的金属箔。
6.一种印刷线路板，所述印刷线路板包含：
一片根据权利要求1至4中任一项所述的预浸料的或两片以上根据权利要求1至4中任一项所述的预浸料的堆叠体的固化产物；和
设置在所述固化产物的一个或两个表面上的导体线路。
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