CN106795307A - 预浸料及覆金属层压板、印刷布线板 - Google Patents

预浸料及覆金属层压板、印刷布线板 Download PDF

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Publication number
CN106795307A
CN106795307A CN201580044726.8A CN201580044726A CN106795307A CN 106795307 A CN106795307 A CN 106795307A CN 201580044726 A CN201580044726 A CN 201580044726A CN 106795307 A CN106795307 A CN 106795307A
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Prior art keywords
resin
prepreg
mass parts
acrylate copolymer
inorganic filler
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CN201580044726.8A
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CN106795307B (zh
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松本匡阳
三户隆人士
米本神夫
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Panasonic Intellectual Property Management Co Ltd
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Panasonic Intellectual Property Management Co Ltd
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Abstract

预浸料具有纤维基材和浸渗于纤维基材的热固化性树脂组合物。热固化性树脂组合物含有：包含环氧树脂的热固化性树脂、固化剂、无机填料和具有10×104以上且不足45×104的重均分子量的丙烯酸酯共聚物。无机填料的含量相对于热固化性树脂与固化剂的合计100质量份为150质量份以上。丙烯酸酯共聚物的含量相对于热固化性树脂与固化剂的合计100质量份为多于30质量份且90质量份以下。

Description

预浸料及覆金属层压板、印刷布线板
技术领域
本发明涉及用于制造印刷布线板的预浸料及覆金属层压板、印刷布线板。
背景技术
印刷布线板被广泛用于电子设备、通信设备、计算机等各种领域。此种印刷布线板通过以下方式来制造，即，将所需片数的预浸料重叠，再配置金属箔，进行加热加压成形使其层叠一体化而制作覆金属层压板，再对表面的金属箔进行图案化加工而使其形成导体布线。上述的预浸料可以通过使包含规定材料的树脂组合物浸渗于玻璃布等纤维基材而得到。
近年来，随着电子技术的迅速发展，电子设备的薄型化·小型化取得进展，随之，需要使印刷布线板具有优异的成形性并且减小翘曲的发生。为了抑制印刷布线板的翘曲的发生，认为降低构成印刷布线板的绝缘层的热膨胀率(CTE：coefficient of thermalexpansion)较为重要。
作为实现绝缘层的低热膨胀率化的方法，可列举例如使构成绝缘层的树脂组合物中以高含有率含有二氧化硅等无机填料的方法。但是，在如上述那样使无机填料高填充化的树脂组合物中存在成形性降低的倾向，并且有对层叠板、印刷布线板的品质造成不良影响的担忧。例如在进行加热加压成形的制造工序中有时发生由树脂组合物(预浸料)中所含的树脂成分与填料的分离所致的条纹不均、或者在绝缘层中产生因局部缺失树脂而成为空隙的飞白(日文原文：力スレ)。
另外，一般而言，若树脂组合物(预浸料)中的无机填料的含量变多，则对树脂固化物(绝缘层)的低CTE化有效，但是浸渗于纤维基材的树脂层反而变脆，在预浸料的表面产生浮粉或在预浸料的端边处理时等容易发生粉粒脱落。即，在使用预浸料制造印刷布线板时，将预浸料切割为规定的尺寸或切掉不需要的边缘后再使用，若树脂组合物中以高含有率包含无机填料，则在切割加工时无机填料、树脂片等的粉屑容易飞散。而且，此种粉屑在之后的成形工序中会附着于预浸料和层叠配置的金属箔的表面等，有在所制造的印刷布线板产生印痕不良的风险。
相反，若树脂组合物中的无机填料的含量变少，则虽然抑制如上所述的粉粒脱落，但是无法得到充分降低CTE的效果。
在专利文献1中公开了在包含环氧树脂和重均分子量为45×104～85×104的丙烯酸类树脂的树脂成分中含有70～90重量％的无机填充材料的复合片。在专利文献1中，通过增大无机填充材料的含有率，从而减小热膨胀系数，并且通过添加丙烯酸类树脂，从而改善复合片的挠性，在片材切割加工时防止切割屑的产生。
现有技术文献
专利文献
专利文献1：日本特开2009-253138号公报
发明内容
本发明提供确保良好的成形性并且能够兼顾抑制粉粒脱落和低CTE化的预浸料及覆金属层压板。
本发明的预浸料具有纤维基材和浸渗于该纤维基材中的热固化性树脂组合物。热固化性树脂组合物含有：包含环氧树脂的热固化性树脂、固化剂、无机填料和具有10×104以上且不足45×104的重均分子量(Mw)的丙烯酸酯共聚物。无机填料的含量相对于热固化性树脂与固化剂的合计100质量份为150质量份以上。丙烯酸酯共聚物的含量相对于热固化性树脂与固化剂的合计100质量份为多于30质量份且90质量份以下。
本发明的覆金属层压板具有绝缘层和设置在该绝缘层上的金属箔，所述绝缘层为上述预浸料的固化物。
在上述预浸料中，热固化性树脂组合物含有相对于热固化性树脂与固化剂的合计100质量份为150质量份以上的无机填料，并且含有多于30质量份且90质量份以下的Mw为10×104以上且不足45×104的丙烯酸酯共聚物。这样，由于在本发明的预浸料中填充有大量的无机填料，因此固化物的CTE变小。另外，由于与无机填料一起并用丙烯酸酯共聚物，因此因丙烯酸酯共聚物所具有的弹性模量而使应力松弛。因此，与仅配合无机填料的情况相比，固化物的CTE进一步变小。进而，通过使丙烯酸酯共聚物的含量为上述的范围，从而无论是否大量含有无机填料，均可抑制在切割时等的粉粒脱落。另外，可以抑制飞白等的发生，从而还可以确保良好的成形性。因此，在使用该预浸料制造的覆金属层压板、印刷布线板中，由于绝缘层的CTE小，因此抑制翘曲的发生，而且还可以防止因预浸料的粉粒脱落所致的印痕不良。
附图说明
图1是本发明的实施方式的预浸料的示意性剖视图。
图2是表示本发明的实施方式的覆金属层压板的一例的示意性截面图。
图3是表示本发明的实施方式的印刷布线板的一例的示意性截面图。
具体实施方式
在说明本发明的实施方式之前，先对以往的复合片、预浸料中存在的问题做简单说明。专利文献1中记载的复合片是不包含纤维基材而与包含纤维基材的预浸料不同的物品。因此，对制造印刷布线板时的成形性等的要求特性也不同。另外，专利文献1所公开的丙烯酸类树脂的重均分子量较大，且配合量也较少。因此，认为难以同时解决预浸料中飞白等成形性和粉粒脱落的问题。
以下，对本发明的实施方式的预浸料进行说明。图1是本实施方式的预浸料10的示意性截面图。预浸料10具有纤维基材4A和浸渗于纤维基材4A的热固化性树脂组合物(以下称为树脂组合物)2A。
树脂组合物2A含有：包含环氧树脂的热固化性树脂、固化剂、无机填料和重均分子量(Mw)为10×104以上且不足45×104的丙烯酸酯共聚物。而且，使树脂组合物2A浸渗于纤维基材4A，并加热干燥至半固化状态(也称作B阶状态)，由此可以形成印刷布线板用的预浸料10。
作为热固化性树脂，可以使用至少包含环氧树脂的树脂。热固化性树脂可以为包含环氧树脂和除其以外的热固化性树脂的混合物，也可以仅包含环氧树脂。
作为环氧树脂，只要是为了形成印刷布线板用各种基板材料而使用的环氧树脂，则并无特别限定。具体而言，可列举：萘型环氧树脂、甲酚酚醛型环氧树脂、双酚A型环氧树脂、双酚F型环氧树脂、双酚S型环氧树脂、脂环式环氧树脂、脂肪族链状环氧树脂、苯酚酚醛型环氧树脂、烷基苯酚酚醛型环氧树脂、芳烷基型环氧树脂、联苯酚型环氧树脂、二环戊二烯型环氧树脂、三羟基苯基甲烷型环氧化合物、酚类与具有酚性羟基的芳香族醛的缩合物的环氧化物、双酚的二缩水甘油基醚化物、萘二醇的二缩水甘油基醚化物、酚类的缩水甘油基醚化物、醇类的二缩水甘油基醚化物、异氰脲酸三缩水甘油酯等。另外，除上述所列举的环氧树脂以外，也可以使用各种缩水甘油基醚型环氧树脂、缩水甘油胺环氧树脂、缩水甘油基酯型环氧树脂、氧化型环氧树脂，此外，还可以使用磷改性环氧树脂等。环氧树脂可以单独使用1种，也可以并用2种以上。由此，从使固化性优异的方面出发，优选使用在1分子中具有2个以上环氧基的环氧树脂。
在热固化性树脂中包含除环氧树脂以外的热固化性树脂的情况下，其种类并无特别限制。可列举例如多官能氰酸酯树脂、多官能马来酰亚胺-氰酸酯树脂、多官能性马来酰亚胺树脂、不饱和聚苯醚树脂、乙烯酯树脂、脲树脂、邻苯二甲酸二烯丙酯树脂、三聚氰胺树脂、胍胺树脂、不饱和聚酯树脂、三聚氰胺-脲共缩合树脂等。这些除环氧树脂以外的热固化性树脂可以单独使用1种，也可以并用2种以上。
固化剂可以使用一直以来一般所使用的固化剂，只要根据热固化性树脂的种类进行适当选定即可。由于在热固化性树脂中包含环氧树脂，因此只要是能够作为环氧树脂的固化剂使用的固化剂，则并无特别限制。可列举例如二胺系固化剂、2官能以上的固化剂等。作为二胺系固化剂，可以使用伯胺、仲胺。作为2官能以上的固化剂，可列举2官能以上的酚化合物、酸酐系固化剂、双氰胺、聚苯醚化合物(PPE)等。这些固化剂可以单独使用1种，也可以并用2种以上。
作为固化剂，特别优选使用2官能以上的酚醛树脂。作为此种2官能以上的酚醛树脂，可列举例如线性酚醛树脂、萘型酚醛树脂、甲酚线性酚醛树脂、芳香族烃甲醛树脂改性酚醛树脂、二环戊二烯酚加成型树脂、苯酚芳烷基树脂、甲酚芳烷基树脂、萘酚芳烷基树脂、联苯改性苯酚芳烷基树脂、苯酚三羟甲基甲烷树脂、四羟苯基乙烷树脂、萘酚线性酚醛树脂、萘酚-苯酚共缩线性酚醛树脂、萘酚-甲酚共缩线性酚醛树脂、联苯改性酚醛树脂、氨基三嗪改性酚醛树脂、联苯酚、乙二醛四苯酚树脂、双酚A线性酚醛树脂、双酚F线性酚醛树脂等。它们可以单独使用1种，也可以并用2种以上。
树脂组合物2A为了降低其固化物的CTE而以较高的含有率包含无机填料。作为无机填料的具体含量，相对于热固化性树脂与固化剂的合计100质量份为150质量份以上。为了进一步降低CTE，优选为200质量份以上。含有越多无机填料，越能期待降低CTE。但是，若无机填料的含量增加，则树脂组合物2A中的树脂成分比率降低。随之，加热成形时的熔融树脂的流动性降低，容易发生飞白、树脂分离等，成形性降低，存在粉粒脱落的风险。
因此，无机填料可容许的含量存在限度，认为：在以往的树脂组合物的树脂设计的范围内，相对于树脂成分100质量份，无机填料的一般的上限为400质量份左右。在本实施方式的情况下，从成形性的观点出发，无机填料的含量的上限也优选为400质量份以下，更优选为360质量份以下。予以说明，在本实施方式中，通过使树脂组合物2A含有丙烯酸酯共聚物，从而还具有提高成形性的效果，因此，无机填料的含量有可能多于400质量份且达到450～500质量份。
无机填料的种类并无特别限定。可以使用例如氧化硅、硫酸钡、氧化硅粉、破碎二氧化硅、烧成滑石、钼酸锌处理滑石、钛酸钡、氧化钛、粘土、氧化铝、云母、勃姆石、硼酸锌、锡酸锌、其他金属氧化物或金属水合物、以及氢氧化铝、碳酸钙、氢氧化镁、硅酸镁、玻璃短纤维、硼酸铝晶须、碳酸硅晶须等。它们可以单独使用1种，也可以并用2种以上。无机填料的形状和尺寸并无特别限制，例如也可以并用不同尺寸的无机填料。从提升无机填料的填充率的观点出发，例如优选并用粒径1μm以上的填料和粒径不足1μm的纳米级的微小填料。也可以利用偶联剂等对这些无机填料实施表面处理。
从降低树脂组合物2A的固化物的CTE并且确保良好的电气性能、耐热性、导热性等其他特性的观点出发，无机填料优选包含二氧化硅。此时，二氧化硅的含量相对于无机填料的总质量适宜为过半量，特别优选为80质量％以上。
树脂组合物2A包含Mw为10×104以上且不足45×104的丙烯酸酯共聚物。此种丙烯酸酯共聚物在对树脂组合物2A的固化物施加因热膨胀所致的应力时发挥缓和该膨胀的作用(膨胀缓和作用)。一般而言，丙烯酸类橡胶粒子等在树脂组合物中以粒状形态存在。另一方面，丙烯酸酯共聚物与丙烯酸类橡胶粒子等不同，在有机溶剂中与其他树脂成分一起制成树脂清漆时，会以不定形且与其他树脂成分相容的状态混合。
丙烯酸酯共聚物由至少包含来自丙烯酸酯的重复构成单元(丙烯酸酯单元)的分子形成。来自丙烯酸酯的重复构成单元是指在使丙烯酸酯单体聚合时所形成的重复构成单元。丙烯酸酯共聚物的分子中包含来自不同的多种丙烯酸酯的重复构成单元，而且还可包含来自除丙烯酸酯以外的单体的重复构成单元。或者，丙烯酸酯共聚物的分子可以由来自不同的多种丙烯酸酯的重复构成单元构成。另外，丙烯酸酯共聚物可以包含来自1种丙烯酸酯的重复构成单元和来自除该丙烯酸酯以外的单体的重复构成单元。
在丙烯酸酯中，作为与酯键中的碳直接键合的取代基，可列举烷基或取代烷基。在取代烷基中，烷基的任意氢原子被其他官能团取代。在为烷基的情况下，可以为直链状，也可以具有支链，另外还可以为脂环式烷基。此外，上述取代基可以为芳香族。作为丙烯酸酯的具体例，可列举丙烯酸甲酯、丙烯酸乙酯、丙烯酸丙酯、丙烯酸异丙酯、丙烯酸丁酯、丙烯酸异丁酯、丙烯酸叔丁酯、丙烯酸戊酯、丙烯酸己酯、丙烯酸环己酯、丙烯酸辛酯、丙烯酸癸酯、丙烯酸月桂酯、丙烯酸苄酯等，但是并不限定于这些例子。
作为除丙烯酸酯以外的单体，可例示为丙烯腈。另外，除此以外，还可列举丙烯酰胺、丙烯酸、甲基丙烯酸、甲基丙烯酸酯、苯乙烯、乙烯、丙烯、丁二烯等除丙烯酸酯以外的乙烯基系单体。在丙烯酸酯共聚物中可以包含来自不同的2种以上的除丙烯酸酯以外的单体的重复构成单元。
构成丙烯酸酯共聚物的重复构成单元可以无规地排列，也可以按照同种的重复构成单元作为嵌段来构成。即丙烯酸酯共聚物可以为无规共聚物，也可以为嵌段共聚物。另外，只要为不阻碍其效果的程度，则丙烯酸酯共聚物可以为具有支链的接枝共聚物，也可以为交联体。
丙烯酸酯共聚物例如可以通过使规定的单体进行自由基聚合而得到，但是并不限定于此种制造方法。
丙烯酸酯共聚物也可以进一步在聚合物分子的末端、侧链或主链具有官能团。该官能团特别优选为与环氧树脂及固化剂中的至少任一者具有反应性的官能团。作为此种官能团，可例示为例如环氧基、羟基、羧基、氨基、酰胺基。通过使上述官能团键合于丙烯酸酯共聚物，从而例如能够与树脂组合物2A中所含的其他成分反应，而被组入热固化性树脂的固化系结构中。因此，耐热性、相容性、耐化学品性等性能提高。在上述列举的官能团中，特别优选环氧基。每1分子聚合物，可以具有多个官能团。予以说明，也将具有如上所述的官能团称作被如上所述的官能团改性，例如将具有环氧基称作环氧改性。
特别优选使丙烯酸酯共聚物具有显示橡胶弹性的分子结构。此时，可以进一步提高膨胀缓和作用的效果。例如包含来自丙烯酸丁酯的重复构成单元和来自丙烯腈的重复构成单元的丙烯酸酯共聚物显示橡胶弹性。另外，此时，即使包含来自丁二烯的重复构成单元，也显示橡胶弹性。
丙烯酸酯共聚物可溶于有机溶剂，与树脂组合物2A的其他成分在有机溶剂中混合而制备树脂清漆时，与可溶于溶剂的其他树脂成分均匀混合。该丙烯酸酯共聚物(以下称为丙烯酸类树脂)可以将固体状的物质在清漆制备时溶解于有机溶剂后再使用，也可以预先制成溶解于有机溶剂的液状后再使用。这样，通过将丙烯酸类树脂溶解于有机溶剂而与其他树脂成分均匀混合，从而容易发挥上述膨胀缓和作用。另外认为容易抑制在加热成形时的流动状态下树脂成分与填料分离的情况。作为有机溶剂，可例示为：丙酮、甲乙酮、环己酮等酮系溶剂；甲苯、二甲苯等芳香族系溶剂；乙酸乙酯等酯系溶剂等。这些有机溶剂可以单独使用1种，也可以并用2种以上。
通过使丙烯酸酯共聚物包含树脂组合物2A，从而容易适当地控制树脂组合物2A的粘度。因此，在由树脂组合物2A形成的基板材料(预浸料10、后述的覆金属层压板20)中，容易发生来自树脂组合物2A的树脂成分与无机填料的分离，使成形性良好。另外，通过使丙烯酸酯共聚物包含树脂组合物2A，从而还能够降低预浸料的CTE。这是由于：通过发挥由丙烯酸酯共聚物带来的上述膨胀缓和作用，从而使热膨胀被丙烯酸酯共聚物吸收。
丙烯酸酯共聚物的Mw为10×104以上且不足45×104，优选为10×104以上且35×104以下。通过使该Mw为该范围，从而如后述那样以相对于热固化性树脂与固化剂的合计100质量份为多于30质量份的量进行配合，可以确保良好的成形性。由此，可以确保良好的成形性，并且可以兼顾抑制切割预浸料10时的粉粒脱落和降低树脂组合物2A的固化物的CTE。另外，容易适合取得在有机溶剂中的溶解性、其配合量与树脂组合物2A的熔融粘度的调整之间的平衡。这样，若使用分子量较小的丙烯酸酯共聚物，则与使用45×104以上的分子量较大的丙烯酸酯共聚物的情况相比，即使大量含有无机填料，也可以抑制树脂组合物2A的熔融粘度的过度上升。若丙烯酸酯共聚物的Mw为45×104以上，则在增多配合量时产生飞白等，存在降低成形性的风险。因此，对丙烯酸酯共聚物的配合量的增多存在限制，难以兼顾低CTE化和确保成形性。另一方面，若丙烯酸酯共聚物的Mw小于10×104，则由丙烯酸酯共聚物产生的弹性变低，存在对低CTE化的贡献降低的风险。另外，还存在无法充分得到预浸料10的防止粉粒脱落的效果。予以说明，此处所说的Mw是指例如利用凝胶渗透色谱进行聚苯乙烯换算而测定得到的值。
只要不阻碍本发明效果，则树脂组合物2A还可以根据需要包含除热固化性树脂、固化剂、无机填料、丙烯酸酯共聚物以外的其他成分。作为其他成分，可以配合例如稀释用的有机溶剂、咪唑等固化促进剂、抗氧化剂、用于提高无机填料的混合性的湿润分散剂、偶联剂、光稳定剂、粘度调节剂、阻燃剂、着色剂、消泡剂等。作为稀释用的有机溶剂，使用例如：丙酮、甲乙酮、环己酮等酮系溶剂；甲苯、二甲苯等芳香族系溶剂；二甲基甲酰胺等含氮溶剂等。
树脂组合物2A可以通过在有机溶剂中分别配合包含环氧树脂的热固化性树脂、固化剂、无机填料、丙烯酸酯共聚物以及根据需要适当添加的添加剂等其他成分来制备。
丙烯酸酯共聚物的含量相对于热固化性树脂与固化剂的合计100质量份为多于30质量份且90质量份以下。如上所述，一般而言，越增加树脂组合物中的无机填料的含量，越能降低固化物的CTE，但是反而处于容易发生粉粒脱落这样的折衷(Trade-off)的关系中。因此，为了兼顾低CTE和抑制粉粒脱落，仅使用无机填料作为低CTE的手段时，存在限度。对此，在本实施方式中，通过在上述的含量的范围内同时含有无机填料和丙烯酸酯共聚物，从而可以利用这些协同效果实现进一步的低CTE化。另外，同时，即使在无机填料为150质量份以上的高含量的情况下，也能抑制粉粒脱落。若丙烯酸酯共聚物的含量为30质量份以下，则存在抑制预浸料的粉粒脱落的效果降低的风险，并且对低CTE化的贡献也变低。另一方面，若丙烯酸酯共聚物的含量大于90质量份，则存在在成形时产生飞白等的风险。
预浸料10可以通过使树脂组合物2A浸渗于纤维基材4A并对其加热干燥至达到半固化状态(B阶状态)来形成。成为半固化状态时的温度条件、时间可以设定为例如120～190℃、3～15分钟。
作为纤维基材4A，并无特别限定，可以使用如平织等那样以使纵线及横线大致正交的方式交织成的基材。可以使用例如如玻璃布等那样的无机纤维织布、如芳纶布、聚酯布等那样的由有机纤维形成的纤维基材。纤维基材4A的厚度并无特别限制，但优选为10～200μm。
以下对本实施方式的覆金属层压板进行简单说明。图2为表示本实施方式覆金属层压板20的一例的示意性剖视图。
覆金属层压板20可以通过取1张预浸料10或将多张重叠并将金属箔14重叠在其双面或单面、再加热加压成形使其层叠一体化来制作。即，覆金属层压板20具有绝缘层12和设置在绝缘层12上的金属箔14，所述绝缘层12为预浸料10的固化物。作为金属箔14，可以使用例如铜箔等。覆金属层压板20例如可以通过使用多段真空压机、双带压机等对预浸料10与金属箔14的层叠体进行加热、加压而成形。
以上那样形成的预浸料10、覆金属层压板20是使用树脂组合物2A来形成的，因此如上述那样具有低CTE，而且不易发生粉粒脱落。因此，在此种预浸料10中不易发生翘曲。另外，还不易发生树脂成分与无机填料的分离(树脂分离)、飞白，在切割时树脂成分及无机填料的粉屑几乎不会飞散。因此，可以有效地被用作用于制作没有成为粉屑附着的主要原因的印痕不良的高性能的印刷布线板的基板材料。
以下，对本实施方式的印刷布线板进行简单说明。图3为表示本实施方式的印刷布线板30的一例的示意性剖视图。
印刷布线板30通过将覆金属层压板20的金属箔14进行加工而设置导体图案16来形成。即，印刷布线板30具有绝缘层12和设置在绝缘层12上的导体图案16，所述绝缘层12为预浸料10的固化物。导体图案16例如可以利用减去(subtractive)法等来形成。另外，之后，在印刷布线板30上安装半导体元件进行密封，由此可以制造FBGA(Fine pitch Ball GridArray)等封装体。另外，使用此种封装体作为子封装体，并将多个子封装体层叠，由此也可以制造PoP(Package on Package)等封装体。
印刷布线板30由低CTE且粉粒不易脱落的基板材料构成。因此，在印刷布线板30上不易发生翘曲，并且几乎未出现印痕不良。
以下，使用更具体的例子说明本实施方式的效果。
准备下述所示的热固化性树脂、固化剂、无机填料、丙烯酸酯共聚物、添加剂(分散剂、偶联剂、抗氧化剂)，将这些原料按照(表1)、(表2)所示的配合量(质量份)进行混合，由此制备树脂清漆(热固化性树脂组合物)。各原料的详细内容如下所述。
<热固化性树脂>
■多官能环氧树脂(日本化药株式会社制“EPPN-502H”)
<固化剂>
■萘骨架酚醛树脂(DIC株式会社制“HPC-9500”)
■苯酚线性酚醛树脂(DIC株式会社制“TD-2090”)
予以说明，上述2种固化剂均为2官能以上的酚醛树脂。
<丙烯酸酯共聚物>
■丙烯酸酯共聚物(环氧改性丙烯酸类树脂、Nagase ChemteX株式会社制“SG-P3mw1”、Mw：25×104)
■丙烯酸酯共聚物(环氧改性丙烯酸类树脂、Nagase ChemteX株式会社制“SG-P3”、Mw：85×104)
<无机填料>
■二氧化硅A(株式会社Admatechs制“SC-4500SQ”)
■二氧化硅B(株式会社Admatechs制“SC-2500SEJ”)
■氢氧化镁(堺化学工业株式会社制“MGZ-6R”)
<添加剂>
■分散剂(BYK-CHEMIE·JAPAN株式会社制“W903”)
■偶联剂(信越硅酮株式会社制“KBE-9007”)
■抗氧化剂(三光株式会社制“HCA”)
使按照(表1)、(表2)所示的配合组成制备的树脂清漆以固化后的厚度达到100μm的方式浸渗于作为纤维基材的玻璃布(日东纺绩株式会社制“2117”、厚度95μm)中，之后，在145℃加热干燥2分钟直至达到半固化状态，由此制造预浸料。
将上述的预浸料重叠4张，并在其双面层叠作为金属箔的厚度12μm的铜箔，边在真空条件下以6.0MPa进行加压，边在200℃加热120分钟进行成形。这样，制造作为覆金属层压板的覆铜层压板。
使用这样制作的各样品的预浸料或覆铜层压板，评价各种物性(粉粒脱落、飞白、CTE)。在(表1)、(表2)中还一并示出各样品的物性评价的结果。
予以说明，各种物性的评价按照以下所示的方法进行。
<粉粒脱落>
通过目视观察利用切割器具切割各样品的预浸料时有无粉粒脱落。
<飞白>
利用蚀刻除去各样品的覆铜层压板的表面的铜箔，目视观察有无表面的飞白，将无飞白的情况判定为“OK”，将有飞白的情况判定为“NG”。
(CTE(拉伸))
对利用蚀刻除去各样品的覆铜层压板的表面的铜箔所得的评价用检品，测定在不足绝缘层中的树脂固化物的玻璃化转变温度的温度下的纵向的热膨胀系数。测定依据基于JIS C 6481(相当于IPC-TM-650 2.4.24.5)的TMA法(Thermo-mechanical analysis)进行，测定中使用热分析装置(Seiko Instruments Inc.公司制“TMA/SS6000”)。
【表1】
phr：perhundred resin(相对于100质量份的树脂的质量份)
【表2】
与(表2)所示的样品CD相比，(表1)所示的样品EA～EC的CTE的值均低，并且均未出现粉粒脱落和飞白。与样品CE相比，样品ED的CTE的值也低，并且也未出现粉粒脱落和飞白。
尤其，若对除丙烯酸酯共聚物以外的组成相同的样品EA～EC进行对比，则可知：丙烯酸酯共聚物的含量越多，对低CTE越有效。
另一方面，在样品CA中，未出现飞白，但是，由于丙烯酸酯共聚物的含量少，因此出现粉粒脱落，CTE也高。另外，在样品CB中，未出现粉粒脱落，但是，由于丙烯酸酯共聚物的含量多，因此出现飞白，无法得到良好的样品片，无法对CTE进行测定。使用重均分子量大的丙烯酸酯共聚物的样品CC虽然未出现粉粒脱落，但是产生飞白。
由以上可知：在样品EA～EC中，使用本实施方式的树脂组合物2A来形成预浸料、覆金属层压板，因此可以维持低CTE，并且可以抑制粉粒脱落。因此，可以制作不易发生翘曲、无印痕不良的高品质的印刷布线板。
产业上的可利用性
可以由本发明的基板材料(预浸料及使用其的覆金属层压板)制作印刷布线板。该印刷布线板由低CTE且不易发生粉粒脱落的基板材料构成。因此，在印刷布线板中不易发生翘曲，几乎未出现印痕不良。因此，更容易应对以薄型化、小型化为目的的电子设备等。因此，这样形成的印刷布线板可以用于例如通信·测量设备、OA设备及其周边终端机等各种用途。
符号说明
2A 热固化性树脂组合物(树脂组合物)
4A 纤维基材
10 预浸料
12 绝缘层
14 金属箔
16 导体图案
20 覆金属层压板
30 印刷布线板

Claims (6)

1.一种预浸料，其具备纤维基材和浸渗于所述纤维基材的热固化性树脂组合物，
所述热固化性树脂组合物含有：
包含环氧树脂的热固化性树脂、
固化剂、
无机填料、和
具有10×104以上且不足45×104的重均分子量的丙烯酸酯共聚物，
所述无机填料的含量相对于所述热固化性树脂与所述固化剂的合计100质量份为150质量份以上，
所述丙烯酸酯共聚物的含量相对于所述热固化性树脂与所述固化剂的合计100质量份为多于30质量份且90质量份以下。
2.根据权利要求1所述的预浸料，其中，所述丙烯酸酯共聚物具有对所述环氧树脂及所述固化剂中的至少任一者具有反应性的官能团。
3.根据权利要求1所述的预浸料，其中，所述无机填料包含80质量％以上的二氧化硅。
4.根据权利要求1所述的预浸料，其中，所述固化剂为2官能以上的酚醛树脂。
5.一种覆金属层压板，其具备绝缘层和设置于所述绝缘层上的金属箔，所述绝缘层为权利要求1所述的预浸料的固化物。
6.一种印刷布线板，其具备绝缘层和设置于所述绝缘层上的导体图案，所述绝缘层为权利要求1所述的预浸料的固化物。
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