CN104884529A - 树脂组合物及包含其的印刷电路基板用层叠体 - Google Patents
树脂组合物及包含其的印刷电路基板用层叠体 Download PDFInfo
- Publication number
- CN104884529A CN104884529A CN201380068477.7A CN201380068477A CN104884529A CN 104884529 A CN104884529 A CN 104884529A CN 201380068477 A CN201380068477 A CN 201380068477A CN 104884529 A CN104884529 A CN 104884529A
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- Prior art keywords
- epoxy resin
- resin
- weight
- rubber
- type epoxy
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
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Classifications
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- H—ELECTRICITY
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- H05K1/00—Printed circuits
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- H05K1/036—Multilayers with layers of different types
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Abstract
本发明涉及起到印刷电路基板用层叠体的绝缘层的作用且表现出与金属基层的粘接性的树脂组合物,上述树脂组合物包含橡胶改性环氧树脂、环氧树脂、无机填料和固化剂。
Description
技术领域
本发明涉及用于印刷电路基板的层叠体以及用于形成上述层叠体所包含的绝缘层和/或粘接剂层的树脂组合物。
背景技术
印刷电路基板用层叠体包含形成电子电路且搭载半导体等电子元件的印刷电路层、传导由电子元件释放出的热的绝缘层和与绝缘层接触而将热向外部释放的放热层。
对于这样的印刷电路基板用层叠体而言,为了提高热传导性、耐电压性等电气特性,以及弯曲性(弯曲加工性)、冲裁性等成型性,在金属基层(起放热层作用)层叠柔性绝缘膜(起绝缘层作用)来制造,并且为了提高金属基层与绝缘膜之间的粘接力,将热塑性聚酰亚胺或环氧树脂用作粘接剂。
然而,热塑性聚酰亚胺在高温的温度条件下实现固化,但这样的固化条件会引起金属基层的氧化且在制造印刷电路基板时引起PSR(Photo SolderResist(光阻焊剂))产生裂纹(crack),环氧树脂因与绝缘膜的相容性问题而存在粘接性和耐热性降低的问题。
另一方面,为了提高粘接性和成型性,引入了将NBR(丁腈橡胶,acrylonitrile-butadiene rubber)或CTBN(端羧基丁腈,carboxyl terminatedbutadiene acrylonitrile)等橡胶(rubber)与环氧树脂混合来用作粘接剂的技术,但想要得到期望水平的印刷电路基板用层叠体中所要求的耐热性、绝缘性和成型性等仍存在局限。
发明内容
技术课题
为了解决上课问题,本发明的目的是,提供与金属基层具有高粘接性的树脂组合物以及包含上述树脂组合物而具有优异的耐热性、绝缘性、成型性等的印刷电路基板用层叠体。
技术解决方法
为了实现上述目的,本发明提供包含橡胶改性环氧树脂、环氧树脂、无机填料和固化剂的树脂组合物。
其中,上述橡胶改性环氧树脂可以是由如下橡胶改性而成的环氧树脂,所述橡胶选自由丁腈橡胶(NBR)、端羧基丁腈(CTBN)橡胶、端环氧基丁腈(ETBN)橡胶和端胺基丁腈(ATBN)橡胶组成的组。
此外,上述橡胶改性环氧树脂的环氧当量(epoxy equivalent weight)可以为300~500g/eq,重均分子量(Mw)可以为30,000~60,000。
另一方面,本发明提供印刷电路基板用层叠体,其包含金属基层和树脂层,所述树脂层通过在上述金属基层上涂覆上述树脂组合物并使其固化而成。
此外,本发明还提供包含上述印刷电路基板用层叠体的印刷电路基板。
附图说明
图1是图示根据本发明的印刷电路基板用层叠体的截面图。
图2和3是图示根据本发明的印刷电路基板的截面图。
具体实施方式
以下,对本发明进行说明。
1.树脂组合物
本发明的树脂组合物包含橡胶改性环氧树脂、环氧树脂、无机填料和固化剂。
本发明的树脂组合物所包含的橡胶改性环氧树脂(rubber-modified epoxyresin)起到提高树脂组合物的粘接性、耐热性和绝缘性的作用。一般而言,橡胶作为线形结构的高分子物质具有微量的未反应基团。由于这样的橡胶的未反应基团难以参与固化反应而降低固化的橡胶的交联密度,因此其最终成为降低耐热性的原因。由此,本发明的特征在于,使用通过将橡胶与环氧树脂聚合而使橡胶的未反应基团最少化来提高固化反应性的橡胶改性环氧树脂。
这样的本发明的橡胶改性环氧树脂优选为由如下橡胶改性而成的环氧树脂,所述橡胶选自由丁腈橡胶(NBR:acrylonitrile-butadiene rubber)、端羧基丁腈(CTBN:carboxyl terminated butadiene acrylonitrile)橡胶、端环氧基丁腈(ETBN:epoxy terminated butadiene acrylonitrile)橡胶和端胺基丁腈(ATBN:amine terminated butadiene acrylonitrile)橡胶组成的组。其中,橡胶改性环氧树脂更优选为将端羧基丁腈(CTBN)橡胶与苯酚酚醛清漆型环氧树脂聚合而进行改性的树脂或将端羧基丁腈(CTBN)橡胶与双酚A型环氧树脂聚合而进行改性的树脂。
另一方面,在将橡胶和环氧树脂聚合时,反应比率(重量%)没有特别限定,当考虑粘接性、耐热性和固化反应性等时,优选使橡胶与环氧树脂以2:8~6:4的比率进行反应,更优选以3:7的比率进行反应。
优选这样的橡胶改性环氧树脂的环氧当量(epoxy equivalent weight)为300~500g/eq,重均分子量(Mw)为30,000~60,000。这是因为,在使用具有上述范围内的当量和重均分子量的橡胶改性环氧树脂的情况下,可以更加提高树脂组合物的粘接性、耐热性和绝缘性。本发明中的“环氧当量”可定义为1个环氧基团对应的环氧共聚物的分子量。
另一方面,本发明的树脂组合物所包含的橡胶改性环氧树脂的含量没有特别限定,当考虑树脂组合物的物性(粘接性、耐热性、绝缘性等)和制造效率(制造过程和费用)时,以树脂组合物100重量%为基准,优选包含8~16重量%。
本发明的树脂组合物所包含的环氧树脂通过优化树脂组合物的交联成型性,起到使树脂组合物的粘接性、耐热性、绝缘性和环境可靠性稳定的作用。这样的环氧树脂只要是本领域公知的环氧树脂就没有特别限制,优选使用选自由双酚A型环氧树脂、氢化双酚A型环氧树脂、双酚F型环氧树脂、双酚S型环氧树脂、酚醛清漆型环氧树脂、甲酚酚醛清漆型环氧树脂、苯酚酚醛清漆型环氧树脂、双环戊二烯型环氧树脂、三苯甲烷型环氧树脂、萘型环氧树脂、联苯型环氧树脂、氢化联苯型环氧树脂和含磷(P)环氧树脂组成的组中的1种以上。
另一方面,本发明的树脂组合物所包含的环氧树脂的含量没有特别限定,当考虑树脂组合物的物性(粘接性、耐热性、绝缘性等)和制造效率(制造过程和费用)时,以树脂组合物100重量%为基准,优选包含50~65重量%。
本发明的树脂组合物所包含的无机填料起到调节树脂组合物的粘度(提高成型性)并且提高固化后的树脂组合物的热传导率的作用。
这样的无机填料只要是本领域公知的无机填料就没有特别限制,优选使用选自由氧化硅、氧化铝、氧化锌、氮化铝、氮化硅、氮化硼、二氧化硅、滑石、碳酸钙和碳酸镁组成的组中的1种以上。
此外,无机填料优选使用平均粒径为约1μm以下的无机填料。具体而言,更优选使用如下的无机填料:以无机填料100体积%为基准,混合了1μm以下的粒子60~80体积%、大于1μm且5μm以下的粒子20~40体积%。这样的本发明的树脂组合物所包含的无机填料的含量没有特别限定,当考虑树脂组合物的粘度、热传导性、作业性和成型性等时,以树脂组合物100重量%为基准,优选包含5~10重量%。
本发明的树脂组合物所包含的固化剂起到引起上述橡胶改性环氧树脂与环氧树脂的固化反应的作用。这样的固化剂只要是本领域公知的固化剂就没有特别限制,优选使用选自由胺系组成的组中的1种以上。
此外,本发明的树脂组合物所包含的固化剂的含量也没有特别限定,当考虑树脂组合物的固化性(交联密度)、作业性和成型性等时,以树脂组合物100重量%为基准,优选包含20~30重量%。
另一方面,为了提高组合物的固化反应速度,本发明的树脂组合物可以进一步包含固化促进剂。这样的固化促进剂只要是本领域公知的固化促进剂就没有特别限制,优选使用选自由苄基二甲胺、三乙醇胺、三亚乙基二胺、二甲基氨基乙醇、三(二甲基氨基甲基)苯酚等叔胺系;2-甲基咪唑、2-苯基咪唑等咪唑系;三苯基膦、二苯基膦、苯基膦等有机膦系;四苯基磷四苯基硼酸盐、三苯基膦四苯基硼酸盐等四苯基硼酸盐组成的组中的1种以上。
此外,本发明的树脂组合物所包含的固化促进剂的含量也没有特别限定,当考虑树脂组合物的固化反应性、作业性和成型性等时,以树脂组合物100重量%为基准,优选包含1重量%以下,具体而言,优选包含0.001~1重量%。
上述本发明的树脂组合物在不脱离其物性及所发挥的效果的范围内可以进一步包含本领域公知的添加剂(例如,消泡剂、分散剂、粘度调节剂、抗氧化剂等)。
本发明的树脂组合物在需要粘接性和/或绝缘性的地方均可使用,优选用于制造柔性印刷电路基板。
2.印刷电路基板用层叠体及包含其的印刷电路基板
本发明提供包含金属基层(11)和树脂层(12)的印刷电路基板用层叠体(参照图1)。
本发明的印刷电路基板用层叠体所包含的金属基层(11)起到将热向外部释放出的放热层作用。能够用作这样的金属基层(11)的物质没有特别限制,可以使用铝(Al)、铜(Cu)、锡(Sn)、金(Au)、银(Ag)或它们的混合物。其中,当考虑放热性和传导性时,金属基层(11)优选使用铝。
本发明的印刷电路基板用层叠体所包含的树脂层(12)作为在金属基层(11)上涂覆以上说明的树脂组合物并使其固化而成的树脂层,起到绝缘层和粘接剂层的作用。其中,涂覆树脂组合物的方法只要是本领域公知的方法就没有特别限制。此外,固化树脂组合物的条件也没有特别限制,优选在一定压力条件下于160℃以上进行2小时的固化。
这样的树脂层(12)由于由上述树脂组合物形成,因此表现出与金属基层(11)高的粘接力,且耐热性、绝缘性和成型性优异。因此,包含上述树脂层(12)的本发明的印刷电路基板用层叠体能够表现出优异的耐热性、绝缘性和成型性。
另一方面,本发明还提供包含上述印刷电路基板用层叠体的印刷电路基板。具体而言,本发明的印刷电路基板可以形成为如下结构:在起到放热层作用的金属基层(11a)与用于形成电路图案的金属层(11b)之间插入起到绝缘层和粘接剂层作用的树脂层(12)的结构(参照图2);用于提高绝缘性、耐久性和耐热性等的、金属基层(11a)/第1树脂层(12a)/热固性聚酰亚胺膜(13)/第2树脂层(12b)/用于形成电路图案的金属层(11b)的结构(参照图3)。其中,第1树脂层(12a)和第2树脂层(12b)是将本发明的树脂组合物固化而成的,金属基层(11a)和金属层(11b)是由传导性金属形成的,可以为彼此相同的物质或不同的物质。
这样的本发明的印刷电路基板的制造方法没有特别限制,可以如下制造:在上述印刷电路基板用层叠体的树脂层(12或12b)上层叠具有传导性的金属层(11b)后,利用蚀刻等方法来形成电路图案或利用将具有传导性的金属物质喷墨印刷的方法来形成电路图案。
以下,例举实施例来更详细说明本发明。但,下述实施例仅为本发明优选的实施例,本发明不限于下述实施例。
[实施例1~6和比较例1~4]
利用本领域公知的方法制造金属基层(铝箔)/第1树脂层/热固性聚酰亚胺膜/第2树脂层/金属层(铜箔)结构的印刷电路基板。此时,以下述表1中的成分和含量分别制造树脂组合物,然后将其固化来分别形成第1树脂层和第2树脂层。
[表1]
[实验例]
利用如下方法对实施例1~6和比较例1~4的树脂组合物以及利用该树脂组合物制造的各印刷电路基板的物性进行评价,并将结果示于下述表2。
1.涂布性
在金属基层(铝箔)上涂布(涂覆)树脂组合物后,对涂布面评价是否发生鱼眼(Fish eye)、针孔(pin hole)和填料纹理(filler texture)等。
2.固化反应性
在金属基层(铝箔)上涂布(涂覆)树脂组合物后,在30kgf/cm2压力下于190℃进行2小时固化来形成第1树脂层。之后,用肉眼评价所形成的第1树脂层的固化状态以及第1树脂层与金属基层之间的粘接程度(翘起状态)。
3.冲裁加工性(成型性)
应用冲裁重量(Punching Weight)150~200吨对准备的印刷电路基板施加5000次打击,然后测定绝缘层(第1和第2树脂层)和PSR的断裂面,从而进行评价。
4.耐热性
根据IPC TM-6502.4.13评价标准,使准备的印刷电路基板漂浮(floating)在288℃焊料(Solder)中,测定绝缘层(第1和第2树脂层)发生分离现象所经过的时间,从而进行评价。
5.耐电压
根据JIS C 2110评价标准,以绝缘距离40μm在Ф为1英寸的圆形电路和金属基层之间施加电压来测定绝缘层(第1和第2树脂层)的击穿时间,从而进行评价。
6.高温高湿处理后耐电压
将准备的印刷电路基板在85℃且85RH%中放置100小时,然后利用与上述耐电压相同的评价方法进行评价。
7.P/S(粘接性)
根据IPC-TM-6502.4.8的评价标准,以90°方向将形成于印刷电路基板的电路图案拉起,测定电路图案(铜箔)剥离的时间,从而进行评价。
[表2]
观察上述表2可以确认到,由包含橡胶改性环氧树脂的本发明的树脂组合物形成绝缘层和粘接剂层的实施例1~6的印刷电路基板的成型性(冲裁加工性)、耐热性、绝缘性(耐电压)和粘接性优异。
另一方面可以确认到,使用聚酰亚胺树脂组合物的比较例1虽然耐热性、绝缘性和粘接性良好,但在将固化温度设为与本发明的树脂组合物相同的情况下,固化反应性降低(一般的聚酰亚胺树脂组合物的固化温度需要250℃以上的高温)。这样,如果固化反应性降低,则在结果上会表现出耐热性和粘接性不良的结果。
除此之外,可以确认到,使用仅混合了橡胶与环氧树脂的树脂组合物的比较例2~4与本发明的树脂组合物(实施例1~6)相比,耐热性、绝缘性和粘接性降低。
工业可利用性
本发明的印刷电路基板用层叠体将包含橡胶改性环氧树脂的树脂组合物用作绝缘层和/或粘接剂层,从而表现出与金属基层高的粘接性,并且耐热性、绝缘性和成型性等优异。
Claims (11)
1.一种树脂组合物,其包含橡胶改性环氧树脂、环氧树脂、无机填料、和固化剂。
2.根据权利要求1所述的树脂组合物,其特征在于,所述橡胶改性环氧树脂是由如下橡胶改性而成的环氧树脂,所述橡胶选自由丁腈橡胶(NBR)、端羧基丁腈(CTBN)橡胶、端环氧基丁腈(ETBN)橡胶和端胺基丁腈(ATBN)橡胶组成的组。
3.根据权利要求1所述的树脂组合物,其特征在于,所述橡胶改性环氧树脂是将端羧基丁腈(CTBN)橡胶与苯酚酚醛清漆型环氧树脂聚合而成的树脂或者将端羧基丁腈(CTBN)橡胶与双酚A型环氧树脂聚合而成的树脂。
4.根据权利要求1所述的树脂组合物,其特征在于,以全体树脂组合物100重量%为基准,所述橡胶改性环氧树脂包含8~16重量%。
5.根据权利要求1所述的树脂组合物,其特征在于,所述橡胶改性环氧树脂的环氧当量(epoxy equivalent weight)为300~500g/eq,重均分子量(Mw)为30,000~60,000。
6.根据权利要求1所述的树脂组合物,其特征在于,所述环氧树脂为选自由双酚A型环氧树脂、氢化双酚A型环氧树脂、双酚F型环氧树脂、双酚S型环氧树脂、酚醛清漆型环氧树脂、甲酚酚醛清漆型环氧树脂、苯酚酚醛清漆型环氧树脂、双环戊二烯型环氧树脂、三苯甲烷型环氧树脂、萘型环氧树脂、联苯型环氧树脂、氢化联苯型环氧树脂和含磷环氧树脂组成的组中的1种以上。
7.根据权利要求1所述的树脂组合物,其特征在于,所述无机填料为选自由氧化硅、氧化铝、氧化锌、氮化铝、氮化硅、氮化硼、二氧化硅、滑石、碳酸钙和碳酸镁组成的组中的1种以上。
8.根据权利要求1所述的树脂组合物,其特征在于,进一步包含固化促进剂。
9.根据权利要求1所述的树脂组合物,其特征在于,以全体树脂组合物100重量%为基准,包含所述橡胶改性环氧树脂8~16重量%、所述环氧树脂50~65重量%、所述无机填料5~10重量%、和所述固化剂20~30重量%。
10.一种印刷电路基板用层叠体,其包含金属基层和树脂层,所述树脂层通过在所述金属基层上涂覆权利要求1~9中任一项所述的树脂组合物并使其固化而成。
11.一种印刷电路基板,其包含权利要求10所述的印刷电路基板用层叠体。
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PCT/KR2013/008824 WO2014073789A1 (ko) | 2012-11-09 | 2013-10-02 | 수지 조성물 및 이를 포함하는 인쇄 회로 기판용 적층체 |
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CN104987673A (zh) * | 2015-08-05 | 2015-10-21 | 张家港康得新光电材料有限公司 | 一种预浸料用环氧树脂组合物、碳纤维预浸料及碳纤维复合材料 |
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WO2023074646A1 (ja) * | 2021-10-27 | 2023-05-04 | 株式会社レゾナック | 樹脂付き金属箔、プリント配線板及びその製造方法、並びに半導体パッケージ |
CN114702882B (zh) * | 2022-05-20 | 2022-12-06 | 信和新材料(苏州)有限公司 | 石化防腐抗蠕变涂料、其制备方法及应用 |
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US20160150644A1 (en) | 2016-05-26 |
EP2918637A4 (en) | 2016-06-22 |
KR101477353B1 (ko) | 2014-12-29 |
WO2014073789A1 (ko) | 2014-05-15 |
CN104884529B (zh) | 2017-07-07 |
KR20140060065A (ko) | 2014-05-19 |
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