CN1334303A - 用于电子部件的胶粘带 - Google Patents

用于电子部件的胶粘带 Download PDF

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CN1334303A
CN1334303A CN00121676A CN00121676A CN1334303A CN 1334303 A CN1334303 A CN 1334303A CN 00121676 A CN00121676 A CN 00121676A CN 00121676 A CN00121676 A CN 00121676A CN 1334303 A CN1334303 A CN 1334303A
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CN1167763C (zh
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金淳植
张镜浩
陈华一
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Toray Advanced Materials Korea Inc
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SEAHAN INDUSTRY Co Ltd
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Abstract

本发明公开了一种胶粘带,这种胶粘带可将引线框架附近的电子部件,如导线、模衬垫(diepads)及发光板半导体集成块,相互粘接在一起,并具有优良的粘合性、耐热性及电性能。通过在耐热薄膜的一面或两面涂敷粘合剂组合物来制备胶粘带,粘合剂组合物包括:一种丙烯酸树脂,一种由双酚A型环氧树脂与甲酚可溶酚醛环氧树脂或可溶可熔酚醛环氧树脂组成的混合环氧树脂,一种含有至少两个分子内马来酰亚胺基的马来酰亚胺化合物,一种芳香二胺化合物,一种含环氧基的液体硅树脂,及一种有机或无机填充剂并将之干燥。

Description

用于电子部件的胶粘带
本发明涉及一种胶粘带，借助于这种胶粘带可将引线框架(1ead frame)附近的电子部件，如引线、模衬垫(diepads)及发光板半导体集成块，相互粘接在一起。
作为一般树脂封装半导体设备所用的胶粘带的例子，有引线框架固定胶粘带、发光板胶粘带及TAB载体胶粘带。对于引线框架固定胶粘带，它被用于固定引线框架的引线，从而提高引线框架本身及整个半导体装配过程中的生产量和生产率。通常，由引线框架制造者将胶粘带用于引线框架；由半导体装配者将这些用于安装半导体集成块，然后将半导体集成块用树脂封装。对于这些功能，用于固定引线框架的胶粘带必须具有优良的可靠性、粘接时的可使用性及使用后的粘合性，同时还须表现出足够的耐热性，以克服半导体设备装配过程中的加热。
用于这些目的的常规胶粘带的例子包括这样的胶粘带，其中聚丙烯腈、聚丙烯酸酯、丙烯腈-丁二烯共聚物，无论是单独或与热固性树脂一起，被涂敷在耐热性支撑薄膜上，如聚酰亚胺薄膜上。最近，由于半导体设备中的多针结构和热辐射的需要，导致了半导体设备的插件结构变得复杂了，也导致对用于胶粘带的有机材料在电的、物理的、热的性能方面及处理方面有了更严格的要求。一般的胶粘带不能满足足够的耐热性、尺寸稳定性及电性能的要求。特别是，当通过一般的绝缘胶粘带，将导线插头粘接到散热片或连接到半导体集成块上时，就会出现严重问题—金属材料，如引线框架，被弯曲或被损坏。
为解决这些问题，美国专利第5494757号及第5500149号公开了液体粘合剂，这种液体粘合剂由一种含有哌嗪基乙基氨基羰基的二丁烯-丙烯腈共聚物和一种至少具有两个马来酰亚胺基团的化合物组成，并可任意地与一种含有二元胺的聚硅氧烷化合物结合。这些液体粘合剂可在相对较低的温度下粘接和固化，同时具有足够的耐热性和电性能，但却遇到一个重大问题—产生大量的溢出气体或差的耐吸湿性。
发明概述
本发明的一个目的是克服现有技术中遇到的问题，提供一种合适的胶粘带用于电子部件的固定。这种胶粘带可在相对较低的温度下粘接和固化，并在耐热性、电性能、耐吸湿性及溢出气体的产生方面都是优良的。
根据本发明，上述目的可通过提供一种胶粘带来实现，这种胶粘带是以一种耐热薄膜为基础的，耐热薄膜一面或两面上的粘合剂组合物包括：100份重的丙烯酸树脂，平均分子量范围是100000-2000000，至少包含一个官能团，这个官能团可以是羧基、醇基、磺酰基、缩水甘油基、氨基；20-500份重的双酚A型环氧树脂；10-200份重的甲酚可溶酚醛环氧树脂或可溶可熔酚醛环氧树脂；10-200份重的马来酰亚胺化合物，其中含有至少两个分子内马来酰亚胺基；一种芳香二胺化合物；及一种含环氧基的液体硅树脂。
发明详述
本发明提供一种粘合剂组合物包含一种丙烯酸树脂(组分A)，一种由双酚A型环氧树脂和甲酚可溶酚醛环氧树脂或可溶可熔酚醛环氧树脂混合而成的混合环氧树脂(组分B)，一种双马来酰亚胺化合物(组分C)，一种芳香二胺化合物(组分D)，一种含环氧基的液体硅树脂(组分E)，一种有机的或无机的填充剂(组分F)。
本发明所用的丙烯酸树脂(组分A)，重均分子量范围是100000-2000000，玻璃体转化温度范围是～50-150℃，并包含至少一个官能团，这个官能团可以是羧基、醇基、磺酰基、缩水甘油基、氨基。例如，如果重均分子量低于100000，那么所合成的粘合剂组合物的热稳定性、粘合性、耐热性就差；另一方面，如果重均分子量超过2000000，那么溶解度很差，致使溶液如此之粘，不能容易地加工处理。
丙烯酸树脂是通过一种混合物的共聚来制备的。这种混合物的组成是：10-60％重量的丙烯腈；20-80％重量的烷基丙烯腈，其烷基部分含有2-12个碳原子；0.1-20％重量的单体，此单体具有一个双键，双键上至少有一个官能团，这个官能团可以是羧基、醇基、磺酰基、缩水甘油基、氨基。当含有官能团的单体低于0.1％的重量时，会给粘合性、耐热性造成有害的影响；当单体高于20％的重量时，其溶液状态的稳定性就差。
至于本发明所用的混合环氧树脂(组分B)，是由双酚A型环氧树脂与甲酚可溶酚醛环氧树脂的混合物，或由双酚A型环氧树脂与可溶可熔酚醛环氧树脂的混合物来制备的。以100份重的组分A为基准，加入20-500份重，最好是80-200份重的双酚A型环氧树脂；加入10-200份重，最好40-100份重的甲酚可溶酚醛环氧树脂或可溶可熔酚醛环氧树脂。如果加入的双酚A型环氧树脂的量低于20份重，则反应产物的粘合性就差；另一方面，如果用太多的双酚A型环氧树脂，则耐热性就不好。如果加入的甲酚可溶酚醛环氧树脂或可溶可熔酚醛环氧树脂低于10份重，则导致反应产物的耐热性的降低；当所用的甲酚可溶酚醛环氧树脂或可溶可熔酚醛环氧树脂超过200份重时，又会产生粘合性方面的问题。
本发明所用的双马来酰亚胺树脂(组分C)是一种化合物，这种化合物具有至少两个分子内马来酰亚胺基团，如下面化学分子式I或II所示：
Figure A0012167600051
以100份重的组分A为基准，优选的使用量大约是10-200份重。例如，当组分C低于10份重，将导致耐热性差、固化后的弹性模量、机械强度的恶化；过量的组分C将降低组合物的粘合性。
与环氧树脂和双马来酰亚胺树脂的用量相比较，组分D(一种芳香二胺化合物)的合适用量是重要的。以100份重的B组分与C组分之和为基准，组分D的优选加入量的范围是1-100份重。组分D加入量的超过或不足，都会导致耐溶剂性、耐热性、耐电性方面的问题。在本发明中，推荐使用在电性能、耐热性、耐化学品性方面突出的芳香二胺化合物。可以使用一种固化剂来促进固化反应。
至于液体硅树脂(组分E)，它具有环氧基团。硅在提供粘合剂内部的化学联结方面，扮演重要的角色。因此，它可使耐热性、耐吸湿性、电绝缘性提高，并由此导致胶粘带耐久性和可靠性的增加。以100份重的组分B为基准，组分E的用量大约为0.1-20份重。例如，不能期望低于0.1份重的组分E会对上述性能有所提高；另一方面，加入量超过20份重，会造成粘合性的降低。
本发明中所用的填充剂(组分F)可以是无机颗粒或有机颗粒。以100份重的组分A为基准，填充剂的用量最好是1-50份重。例如，低于1份重的填充剂将使粘合剂成分太粘，不容易处理，并减低粘合剂的机械强度和弹性模量；另一方面，超过50份重又将导致粘合性问题。氧化锌、二氧化硅、氧化铝、二氧化锆粉末可作为无机填充剂来使用，有机填充剂的例子包括粉末状的丙烯酸树脂、聚酰胺树脂及硅氧烷。
将上述组分A到组分F溶解于一种溶剂，使其粘度为100-2000cps，最好为300-1000cps。
将因此而得到的组合物涂敷于一种耐热性薄膜上，按干燥后的厚度为10-50μm取量。在80-120℃下干燥1-20分钟后，将一释放薄膜施用于支持膜组合物上，并进行胶粘带的通常处理，即在80-120℃下保持1-20分钟完成半固化，以得到用于电子部件的耐热性胶粘带。
本发明中可用的耐热薄膜，可由热树脂如聚酰亚胺、聚苯硫醚、聚对苯二甲酸乙二酯、聚萘二甲酸乙二醇酯来制备。大约5-100μm厚比较好，25-150μm厚更好。
释放薄膜的例子包括聚丙烯薄膜、氟树脂薄膜、聚乙烯薄膜、聚对苯二甲酸乙二酯薄膜和纸。此外，如果需要，可通过使用硅氧烷树脂，使这些树脂提供更好的可释放性。
根据下面的实施例，可对本发明获得更好的理解。这些实施例是对本发明的说明，而不是对本发明限制。
实施例I
由30％重量的丙烯腈、65％重量的丙烯酸丁酯、5％重量的甲基丙烯酸组成单体混合物，可在聚合引发剂存在下，由该单体混合物的共聚来制备丙烯酸树脂。向100份重重均分子量为1000000的这样的丙烯酸树脂中，加入100份重的双酚A型环氧树脂(环氧当量为100)，50份重的甲酚可溶酚醛环氧树脂(环氧当量为200)，25份重的N′，N′-(4，4′-二苯基甲烷)双马来酰亚胺，25份重的二氨基二苯基甲烷，2份重的含有环氧基团的液体硅树脂，6份重的平均粒度为2.0μm的氧化锌；随后加入甲乙酮和甲苯，得到一粘性溶液，其粘度范围为从800到1000cps。
在50μm厚的聚酰亚胺薄膜上，如Du Pont出售的商标名为“KAPTON”的薄膜，涂敷足够厚的该粘性溶液，以保证干燥后涂层的厚度为20μm。在120℃下干燥5分钟，然后用38μm厚的聚对苯二甲酸乙二醇酯薄膜覆盖在涂层上，即得胶粘带。
实施例II
由30％重量的丙烯腈、65％重量的丙烯酸丁酯、5％重量的丙烯酸缩水甘油酯组成单体混合物，可在聚合引发剂存在下，由该单体混合物的共聚来制备丙烯酸树脂。将100份重重均分子量为1200000的这样的丙烯酸树脂，200份重的双酚A型环氧树脂，100份重的甲酚可溶酚醛环氧树脂，50份重的N′，N′-(4，4′-二苯基甲烷)双马来酰亚胺，50份重的二氨基二苯基甲烷，2份重的含有环氧基团的液体硅树脂，6份重的平均粒度为2.0μm的氧化锌，互相混合并溶解于甲乙酮和甲苯中，得到一粘性溶液，其粘度范围为从800到1000cps。使用这种粘性溶液，按与实施例I相同的方法，即可制得一种胶粘带。
实施例III
由40％重量的丙烯腈、52％重量的丙烯酸丁酯、3％重量的甲基丙烯酸羟乙酯和5％重量的丙烯酸缩水甘油酯组成单体混合物，可在聚合引发剂存在下，由该单体混合物的共聚来制备丙烯酸树脂。将100份重重均分子量为900000的这样的丙烯酸树脂，200份重的双酚A型环氧树脂，100份重的甲酚可溶酚醛环氧树脂，50份重的N′，N′-(4，4′-二苯基甲烷)双马来酰亚胺，50份重的二氨基二苯基甲烷，2份重的含有环氧基团的液体硅树脂，6份重的平均粒度为2.0μm的氧化锌，互相混合并溶解于甲乙酮和甲苯中，得到一粘性溶液，其粘度范围为从800到1000cps。使用这种粘性组合物，按与实施例I相同的方法，即可制得一种胶粘带。
对比例I
由30％重量的丙烯腈、65％重量的丙烯酸丁酯、5％重量的甲基丙烯酸组成单体混合物，可在聚合引发剂存在下，由该单体混合物的共聚来制备丙烯酸树脂。将100份重重均分子量为1200000的这样的丙烯酸树脂，300份重的双酚A型环氧树脂，50份重的二氨基二苯基甲烷，2份重的含有环氧基团的液体硅树脂，6份重的平均粒度为2.0μm的氧化锌，互相混合并溶解于甲乙酮和甲苯中，得到一粘性溶液，其粘度范围为从800到1000cps。使用这种粘性组合物，按与实施例I相同的方法，即可制得一种胶粘带。
对比例II
由30％重量的丙烯腈、65％重量的丙烯酸丁酯、5％重量的甲基丙烯酸组成单体混合物，可在聚合引发剂存在下，由该单体混合物的共聚来制备丙烯酸树脂。将100份重重均分子量为1200000的这样的丙烯酸树脂，200份重的双酚A型环氧树脂，100份重的甲酚可溶酚醛环氧树脂，50份重的N′，N′-(4，4′-二苯基甲烷)双马来酰亚胺，50份重的二氨基二苯基甲烷，6份重的平均粒度为2.0μm的氧化锌，互相混合并溶解于甲乙酮和甲苯中，得到一粘性溶液，其粘度范围为从800到1000cps。使用这种粘性组合物，按与实施例I相同的方法，即可制得一种胶粘带。
对比例III
由40％重量的丙烯腈、60％重量的丙烯酸丁酯组成单体混合物，可在聚合引发剂存在下，由该单体混合物的共聚来制备丙烯酸树脂。将100份重平均分子量为1000000的这样的丙烯酸树脂，50份重的双酚A型环氧树脂，200份重的甲酚酚醛环氧树脂，50份重的N′，N′-(4，4′-二苯基甲烷)双马来酰亚胺，50份重的二氨基二苯基甲烷，2份重的含有环氧基团的液体硅树脂，6份重的平均粒度为2.0μm的氧化锌，互相混合并溶解于甲乙酮和甲苯中，得到一粘性溶液，其粘度范围为从800到1000cps。使用这种粘性组合物，按与实施例I相同的方法，即可制得一种胶粘带。
采用下述方法，对从实施例和对比例中得到的胶粘带，进行各种性能测试，测试结果见于下面表1。
粘合性
将一薄铜片置于保持在150℃加热板上，然后通过使用胶粘带，在铜片上以5 Kg/cm2的压力作用0.5秒。在175℃的热鼓风炉中干燥1小时后，就可使用张力强度测定仪，测量胶粘带的T-剥离强度。
热解温度
使用热重力分析仪(Du Pont V4，IC2200)，测量胶粘带损失其重量的5％时的温度。
溢出气体
在170℃的干燥器中保存1小时后，测量胶粘带重量的变化量。
吸湿百分数
在23℃的水中浸泡1小时后，测量胶粘带重量的变化量。
弹性模量
在170℃干燥1小时及在250℃下又干燥1小时后，使用张力强度测定仪，测量胶粘带的弹性模量。
表1
胶粘带 粘合性(g/cm)  热解温度(℃)  溢出气体(％) 吸湿百分数(％) 弹性模量Kg/mm2
实施例I   760     370     0.6     1.5     4120
实施例II   740     395     0.6     1.5     4570
实施例III   920     395     0.7     1.7     4990
对比例I   730     340     1.1     1.6     3650
对比例II   810     390     0.6     2.5     4360
对比例III   250     395     0.6     1.7     4860
总之，从实施例和对比例中得到的数据证明了，按本发明所制备的胶粘带在所有已测试的性能方面都是优良的，其中包括粘合性、耐热性和耐吸湿性；而对比例子中所制备的一般的胶粘带在个别的性能方面是不良的。例如，对比例I的胶粘带，具有产生大量溢出气体和低弹性模量的缺点；对于对比例II，耐吸湿性尤其不良；对比例III的胶粘带，粘合性是不良的。
如上面描述的，按本发明所制备的胶粘带，具有优良的物理性能包括粘合性、耐热性、耐吸湿性等及优良的电性能，因此，它对电子部件如半导体设备将是非常有用的。
已以说明的方式描述了本发明，应当理解所用的术语是为描述而不是为了限制。根据上面的示教，本发明的很多修改和变动是可能的。因此，应当理解，在所附权利要求的范围内，除具体的描述以外，本发明也是可以实施的。

Claims (5)

1、一种胶粘带，由一种作为基膜的耐热薄膜和涂敷于其一面或两面的粘合剂组合物所组成，所说的粘合剂组合物包括：
(A)100份重的重均分子量范围为100000-2000000的丙烯酸树脂，其中包含至少一个官能团，这个官能团可以是羧基、醇基、磺酰基、缩水甘油基、氨基；
(B)20-500份重的双酚A型环氧树脂和10-200份重的甲酚可溶酚醛环氧树脂或可溶可熔酚醛环氧树脂；
(C)10-200份重的马来酰亚胺化合物，这种化合物具有至少两个分子内马来酰亚胺基团；
(D)一种芳香二胺化合物；
(E)一种含环氧基的液体硅树脂。
2、权利要求1的胶粘带，其中的丙烯酸树脂是通过一种混合物的共聚来制备的，这种混合物包含：10-60％重量的丙烯腈；20-80％重量的烷基丙烯腈，其烷基部分含有2-12个碳原子；0.1-20％重量的单体，此单体具有一个双键，双键上至少有一个官能团，这个官能团可以是羧基、醇基、磺酰基、缩水甘油基、氨基。
3、权利要求1的胶粘带，其中组分(C)是一种由下面化学分子式I或II所示的化合物：
4、权利要求1的胶粘带，其中组分(D)的用量为1-100份重量，以组分(B)与组分(C)之和为100份重量作基准。
5、权利要求1的胶粘带，其中组分(E)的用量为0.1-20份重量，以组分(B)为100份重量作基准。
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