CN1931947B - 电路连接用粘合剂组合物 - Google Patents

电路连接用粘合剂组合物 Download PDF

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Publication number
CN1931947B
CN1931947B CN2006101371470A CN200610137147A CN1931947B CN 1931947 B CN1931947 B CN 1931947B CN 2006101371470 A CN2006101371470 A CN 2006101371470A CN 200610137147 A CN200610137147 A CN 200610137147A CN 1931947 B CN1931947 B CN 1931947B
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aqueous
circuit
rubber
binder composition
film
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CN1931947A (zh
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加藤木茂树
须藤朋子
汤佐正己
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Resonac Corp
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Hitachi Chemical Co Ltd
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Abstract

本发明提供的电路连接用粘合剂组合物，是使电路基板的主面上具有电路电极的、对置的电路构件相互间粘合，目的在于使一方的电路构件的电路电极和另一方的电路构件的电路电极形成电连接，该电路连接用粘合剂组合物含有由热塑性树脂、热固性成分、平均粒径1～18μm的导电粒子、含有丙烯腈的共聚物构成的橡胶，其中，相对于电路连接用粘合剂组合物总体积，含有所述导电粒子0.1～30体积％。

Description

电路连接用粘合剂组合物
本申请是原申请的申请日为2003年12月1日，申请号为200380100586.9，发明名称为《粘合剂组合物、电路连接用粘合剂组合物、连接体及半导体装置》的中国专利申请的分案申请。 
技术领域
本发明涉及粘合剂组合物、电路连接用粘合剂组合物、连接体及半导体装置。 
背景技术
在半导体元件和液晶显示元件中，使用各种粘合剂来结合元件中的各种的构件。这样的粘合剂以要求粘合性为首，还要求耐热性、高温高湿状态中的可靠性等涉及多方面的特性。另外，作为在粘合中使用的被粘合体，例如使用印刷配线板或聚酰亚胺等有机基材等具有酮、铝等金属或ITO(铟锡氧化物)、SiN、SiO2等多种多样表面状态的基材，因此配合各被粘合体的分子设计是必要的。 
以往，作为半导体元件或液晶显示元件用的粘合剂，可以采用使用了显示高粘合性和高可靠性的环氧树脂的热固性树脂(例如，特开平1-113480号公报)。作为树脂的构成成分，一般使用环氧树脂、具有和环氧树脂反应性的酚醛树脂等固化剂、促进环氧树脂和固化剂反应的热潜伏性催化剂。热潜伏性催化剂已成为决定固化温度和固化速度的重要因素，从室温(25℃)下的贮存稳定性和加热时的固化速度的观点出发，可以使用各种化合物。在实际操作中，通过在170～250℃的温度下固化1～3小时，就可得到所要求的粘合。但是，随着最近半导体元件的高集成化、液晶元件的高精细化，元件间和配线间的间距更为狭小，因而，固化时的加热对周围构件造成不良影响的危险就出现了。进而为实现低成本化，就有必要提高通过量，要求在低温(100～170℃)、短时间(1小时以内)，换句话说低温快速固化下的粘合。为达到这种低温快速 固化，就需要使用低活化能的低热潜伏性催化剂，但是已经知道，这样的热潜伏性催化剂兼具在室温附近的贮存稳定性是非常困难的。 
最近，并用了(甲基)丙烯酸酯衍生物和作为自由基引发剂的过氧化物的自由基固化型粘合剂正受到关注。自由基固化，作为反应活性种的自由基非常富有反应性，因此短时间固化是可能的，而且可以在低于或等于自由基引发剂的分解温度下稳定地存在，因而是低温快固化和室温附近下的贮存稳定性并立的固化系(例如，特开2002-203427号公报)。 
发明内容
但是，自由基固化系粘合剂，固化时的收缩大，因此与使用环氧树脂时相比，粘合强度差，特别对无机材质或金属材质的基材的粘合强度降低。因此，在用于半导体元件或液晶显示元件的粘合剂时，就得不到足够的性能(粘合强度等)。 
因此，本发明的目的在于，提供虽然是自由基固化系，但对以金属和无机材质构成的基材显示高粘合强度、室温(25℃)下的贮存稳定性优良、而且可靠性试验后具有足够的性能的粘合剂组合物，电路连接用粘合剂组合物，连接体和半导体装置。 
为达到上述目的，本发明提供含有(a)～(d)成分的粘合剂组合物。 
(a)热塑性树脂， 
(b)具有2个或2个以上(甲基)丙烯酰基的自由基聚合性化合物， 
(c)利用150～750nm的光照射和/或80～200℃的加热产生自由基的固化剂(利用150～750nm的光照射，或者80～200℃的加热，或者并用光照射和加热产生自由基的固化剂)， 
(d)其单独时在25℃的粘度是10～1000Pa·s的液状橡胶。 
在该粘合剂组合物中，向含具有(甲基)丙烯酰基的自由基聚合性化合物的自由基固化系的粘合剂组合物中，以赋予薄膜成形性为主要目的，加入热塑性树脂，再调配入上述特定粘度的液状橡胶，由此达到对以金属或无机材质等构成的基材的高粘合强度。另外，(甲基)丙烯酰指的是丙烯酰或者甲基丙烯酰(以下相同)。 
这里，(d)液状橡胶的主骨架，优先从聚异戊二烯、聚丁二烯、苯乙烯- 丁二烯共聚物、丙烯腈-丁二烯共聚物、聚(氧丙烯)、聚(氧四亚甲基)二醇、聚烯烃二醇和聚-ε-己内酯组成的组中选择。即，(d)成分可以是从聚异戊二烯、聚丁二烯、苯乙烯-丁二烯共聚物、丙烯腈-丁二烯共聚物、聚(氧丙烯)、聚(氧四亚甲基)二醇、聚烯烃二醇、聚-ε-己内酯及其改性物组成的组中选择的、单独时在25℃的粘度为10～1000Pa·s的液状橡胶。 
通过使用这些液状橡胶，提高向粘合基材表面的润湿性，能够达到高粘合强度。 
相对于100重量份数(a)成分，粘合剂组合物优先选择含有50～250重量份数(b)成分、0.5～30重量份数(c)成分和1～50重量份数(d)成分。通过形成这样的配合比率，粘合强度、薄膜成形性、耐热性、固化速度、放置稳定性等能够变得更为优良。 
在上述粘合剂组合物中，相对于粘合剂组合物总体积可以含有0.1～30体积％的导电粒子。即，得到相对于粘合剂组合物总量100体积份数，含有0.1～30体积％导电粒子的粘合剂组合物。 
通过在粘合剂组合物中配合导电粒子，粘合剂组合物已经能够作为异向导电性的粘合剂使用。异向导电性的粘合剂组合物，例如在作为连接电路基板的主面上具有电路电极的电路构件相互间的电路连接用粘合剂组合物使用时，在保持同一电路基板上的电路电极间的绝缘性的同时，借助导电粒子能够使对置的电路基板上的电路电极间形成电连接。 
即，提供为实现一方的电路构件的电路电极和另一方的电路构件的电路电极形成电连接而将电路基板的主面上具备电路电极的电路构件相互间对置进行连接的、并由上述粘合剂组合物构成的电路连接用粘合剂组合物。 
该电路连接用粘合剂组合物是，在将电路连接用粘合剂组合物介于具有对置电极的基板间，并向对置的基板间加压从而使加压方向的电极间形成电连接的电路连接方法中，以使用上述粘合剂组合物作为电路连接用粘合剂组合物为特征的电路连接用粘合剂组合物。 
通过使用该电路连接用粘合剂组合物提供下面的连接体及半导体装置。 
一种连接体，其具备：在第一电路基板的主面上具有第一电路电极的第一电路构件，在第二电路基板的主面上具有第二电路电极的第二电路构件， 以及在第一和第二电路电极对置的状态下设置在第一和第二电路构件之间的、使第一和第二电路电极形成电连接的电路连接构件；其中，上述电路连接构件由上述粘合剂组合物或者其固化物构成。 
一种半导体装置，其具备：具有连接电极的半导体元件，在电路基板的主面上具有电路电极的电路构件，以及在连接电极和电路电极对置的状态下设置在半导体元件和电路构件之间的、使连接电极和电路电极形成电连接的电路连接构件；其中，上述电路连接构件由上述粘合剂组合物或者其固化物构成。 
尤其是，通过使用含有导电粒子的电路连接用粘合剂组合物，提供下面的连接体和半导体装置。 
一种连接体，其具备：在第一电路基板的主面上具有第一电路电极的第一电路构件，在第二电路基板的主面上具有第二电路电极的第二电路构件，以及在第一和第二电路电极对置的状态下设置在第一和第二电路构件之间的、使第一和第二电路电极形成电连接的电路连接构件；其中，上述电路连接构件由含有相对于粘合剂组合物总体积的0.1～30体积％的导电粒子的粘合剂组合物或者其固化物构成，利用该粘合剂组合物或者其固化物中的导电粒子，使第一和第二电路电极间形成电连接。 
一种半导体装置，其具备：具有连接电极的半导体元件，在电路基板的主面上具有电路电极的电路构件，以及在连接电极和电路电极对置的状态下设置在半导体元件和电路构件之间的、使连接电极和电路电极形成电连接的电路连接构件；其中，上述电路连接构件由含有相对粘合剂组合物总体积的0.1～30体积％导电粒子的粘合剂组合物或者其固化物构成，利用该粘合剂组合物或者其固化物中的导电粒子，使电极和电路电极间形成电连接。 
附图说明
图1是用不含导电粒子的电路连接用粘合剂组合物连接的、有关实施方式的连接体的剖面图； 
图2是表示第一电路构件、第二电路构件和薄膜状的电路连接用粘合剂组合物(不含导电粒子)的剖面图； 
图3是表示用含有导电粒子的电路连接用粘合剂组合物连接的、有关实 施方式的连接体的剖面图； 
图4是模拟地表示第一电路构件、第二电路构件和薄膜状的电路连接用粘合剂组合物(含导电粒子)的剖面图； 
图5是有关实施方式的半导体装置的斜视图； 
图6是图5的沿VI-VI线的剖面图。 
具体实施方式
作为本发明中使用的(a)成分的热塑性树脂，没有特别的限制，可以使用公知的热塑性树脂。作为这样的聚合物，可以使用聚酰亚胺、聚酰胺、苯氧基树脂类、聚(甲基)丙烯酸酯类、聚酰亚胺类、聚氨酯类、聚酯类、聚乙烯醇缩丁醛类等。这些可以单独使用，也可以将两种或两种以上混合使用。这些树脂中可以含有硅氧烷键或氟取代基。这些混合的树脂相互间如果是在完全相溶，或者是发生微相分离而呈白浊状态，是能够适合使用的。上述树脂的分子量越大，越容易得到薄膜成形性，并且能够将影响作为粘合剂的流动性的熔融粘度设定在宽范围。分子量没有特别的限制，但作为一般的重均分子量优选是5000～150000，尤其优选是10000～80000。在该值不到5000时，有薄膜成形性变差的倾向，另外如果超过150000，就有和其他成分的相溶性变差的倾向。 
作为本发明中使用的(b)成分、并具有2个或2个以上(甲基)丙烯酰基的自由基聚合性化合物，没有特别的限制，可以使用公知的自由基聚合性化合物。 
具体地可举出环氧(甲基)丙烯酸酯低聚物、氨基甲酸酯(甲基)丙烯酸酯低聚物、聚醚(甲基)丙烯酸酯低聚物、聚酯(甲基)丙烯酸酯低聚物等低聚物，三羟甲基丙烷(甲基)丙烯酸酯、聚乙二醇二(甲基)丙烯酸酯、聚亚烷基二醇二(甲基)丙烯酸酯、二环戊烯(甲基)丙烯酸酯、二环戊烯氧基乙基(甲基)丙烯酸酯、新戊二醇二(甲基)丙烯酸酯、二季戊四醇六(甲基)丙烯酸酯、异氰脲酸改性2官能(甲基)丙烯酸酯、异氰脲酸改性3官能(甲基)丙烯酸酯、2，2′-二(甲基)丙烯酰氧基二乙基磷酸酯、2-(甲基)丙烯酰氧基乙基酸性磷酸酯等多官能(甲基)丙烯酸酯化合物。这些化合物，根据需要，可以单独使用或者混合使用。 
(b)成分的添加量，相对于100重量份数的(a)成分，优选是50～250重量 份数，更优选是60～150重量份数。在添加量不到50重量份数时，有固化后的耐热性降低的担心，另外在超过250重量份数时，在作为薄膜使用的情况下，有薄膜成形性降低的危险。 
作为本发明中使用的(c)成分、并利用150～750nm的光照射和/或80～200℃的加热而产生自由基的固化剂，没有特别的限制，可以使用α-乙酰氨基苯酮衍生物或过氧化物、偶氮化合物等公知的固化剂。作为这些化合物，特别从固化温度的设计的容易等方面出发，更优选过氧化物。作为能够使用的过氧化物，以表示过氧化物分解尺度的1分钟的半衰期温度作为参照是简便的，优选1分钟的半衰期温度在40℃～200℃范围，其中更加优选1分钟的半衰期温度在60℃～170℃范围。当1分钟的半衰期温度不到40℃时，往往损害保存稳定性，当超过200℃时，往往需要长时间固化。 
作为这样的固化剂，可举出二酰基过氧化物衍生物、过氧二碳酸酯衍生物、过氧酯衍生物、过氧缩酮衍生物、二烷基过氧化物衍生物、氢过氧化物衍生物。 
作为二酰基过氧化物衍生物，可举出2，4-二氯苯甲酰过氧化物、3，5，5-三甲基己酰基过氧化物、辛酰基过氧化物、月桂酰过氧化物、硬脂酰过氧化物、琥珀酰过氧化物、苯甲酰过氧化甲苯、苯甲酰过氧化物等。 
作为过氧二碳酸酯衍生物，可举出过氧化二碳酸二正丙酯、过氧二碳酸二异丙酯、双(4-叔丁基环己基)过氧二碳酸酯、二-2-乙氧基甲氧基过氧二碳酸酯、二(2-乙基己基过氧)二碳酸酯、过氧二碳酸二甲氧基丁酯、二(3-甲基-3-甲氧丁基过氧)二碳酸酯等。 
作为过氧酯衍生物，可举出1，1，3，3-四甲基丁基过氧新癸酸酯、1-环己基-1-甲乙基过氧新癸酸酯、过氧新癸酸叔己酯、过氧新戊酸叔丁酯、1，1，3，3-四甲丁基过氧-2-乙基己酸酯、2，5-二甲基-2，5-双(2-乙基乙酰基过氧)己烷、2，5-二甲基-2，5-双(2-过氧化苯甲酰)己烷、1-环己基-1-甲乙基过氧-2-乙基己酸酯、叔己基过氧-2-乙基己酸酯、过氧异丁酸叔丁酯、1，1-双(叔丁基过氧)环己烷、叔己基过氧异丙基单碳酸酯、叔丁基过氧-3，5，5-三甲基己酸酯、过氧月桂酸叔丁酯、2，5-二甲基-2，5-二(间甲苯酰基过氧)己烷、叔丁基过氧异丙基单碳酸酯、叔丁基过氧-2-乙基己基单碳酸酯、过氧苯甲酸叔己酯、过乙酸叔丁酯等。 
作为过氧缩酮衍生物，可举出1，1-双(叔己基过氧)-3，3，5-三甲基环己烷、1，1-(叔丁基过氧)环十二烷、2，2-双(4，4-二叔丁基过氧环己基)丙烷、2，2-双(叔丁基过氧)癸烷等。 
作为二烷基过氧化物衍生物，可举出α，α′双(叔丁基过氧)二异丙基苯、二枯烯基过氧化物、2，5-二甲基-2，5-二(叔丁氧基)己烷、叔丁基枯烯基过氧化物等。 
作为氢过氧化物类，可举出二异丙基苯氢过氧化物、枯烯基氢过氧化物等。 
这些化合物除了单独使用以外，也可以将两种或两种以上混合使用。 
(c)成分的添加量，相对于100重量份数的(a)成分，优选是0.5～30重量份数，更优选是1～20重量份数。在添加量不到0.5重量份数时，有固化不足的担心，另外，在超过30重量份数时，有放置稳定性降低的危险。 
作为本发明使用的(d)成分的液状橡胶，可以使用不含溶剂等的、单独时在25℃的粘度是10～1000Pa·s的液状橡胶(优选是50～800Pa·s、更优选是100～500Pa·s、最优选是150～250Pa·s)化合物。该粘度是使用旋转数控制式的旋转粘度计(E型粘度计等)，采用锥型和平板型的几何学，在旋转转数0.5～50r/min、25℃测定的值。如果该粘度不到10Pa·s，在以粘合剂组合物作为薄膜使用时，就有固化后的弹性率显著降低的危险，如果超过1000Pa·s，就有随着薄膜的低流动化，粘合性降低的危险。 
作为这样的液状橡胶，特别优选聚异戊二烯、聚丁二烯、苯乙烯-丁二烯共聚物、丙烯腈-丁二烯共聚物、聚(氧丙烯)、聚(氧四亚甲基)二醇、聚烯烃二醇和聚-ε-己内酯及其改性物。这里所说的改性物是指，通过使具有交联性官能基的单体共聚等，从而在侧链或末端导入了和主结构不同的结构的改性物。 
作为上述的具体的例子，可举出液状聚异戊二烯，液状聚丁二烯，羧基末端液状聚丁二烯，羟基末端液状聚丁二烯，液状1，2-聚丁二烯，羧基末端液状1，2-聚丁二烯，羟基末端液状1，2-聚丁二烯，液状苯乙烯-丁二烯橡胶，羟基末端液状苯乙烯-丁二烯橡胶，液状丙烯腈-丁二烯橡胶，在聚合物末端含有羧基、羟基、(甲基)丙烯酰基或者吗啉基的液状丙烯腈-丁二烯橡胶、液状羧基化丁腈橡胶、羟基末端液状聚(氧丙烯)、烷氧基甲硅烷基末端液状聚(氧 丙烯)、液状聚(氧四亚甲基)二醇、液状聚烯烃二醇、液状聚-ε-己内酯。 
其中，更加优选极性较高的液状丙烯腈-丁二烯橡胶，在聚合物末端含有羧基、羟基、(甲基)丙烯酰基或者吗啉基的液状丙烯腈-丁二烯橡胶，液状羧基化丁腈橡胶，其中，极性基团丙烯腈的含量更优选是10～60％。使用这样的极性高的液状橡胶，能够更提高粘合强度。 
除了单独使用这些化合物以外，也可以将其两种或两种以上混合使用。 
(d)成分的添加量，相对于100重量份数的(a)成分，是1～50重量份数，优选是10～30重量份数。在添加量不到1重量份数时，难以得到高粘合强度，另外，在超过50重量份数时，固化后的粘合剂的物理性能降低显著，有可靠性降低的危险。 
作为本发明中使用的导电粒子，可举出Au、Ag、Ni、Cu、软钎料等的金属粒子或碳黑等。另外，也可以是以非导电性的玻璃、陶瓷、塑料等为核，在该核上被覆金属、金属粒子或碳黑而成的导电粒子。特别地，作为导电粒子，可以使用以塑料为核，并在该核上被覆有上述金属、金属粒子或碳黑的粒子或热熔融金属粒子，加热加压而具有变形性，因此可吸收电极的高度偏差，也可在连接时增加和电极的接触面积从而提高可靠性，因而是优选的。另外，这些导电粒子的表面进而用高分子树脂等所被覆的微粒子，可以抑制增加导电粒子的配合量时的粒子相互间的接触所引起的短路，提高电极电路间的绝缘性，因此可以适宜地单独使用该微粒子或者和导电粒子混合使用。 
该导电粒子的平均粒径，从分散性、导电性方面来看，优选是1～18μm。平均粒径如果不到1μm，则电路电极相互间的电连接往往变得不充分，如果超过18μm，向电极间距离狭小的高密度的电路构件的应用就变得困难。 
导电粒子的使用量没有特别的限制，但相对于粘合剂组合物总体积，优选是0.1～30体积％，更优选是0.1～10体积％。该值如果不到0.1体积％，就有导电性变差的倾向，如果超过30体积％，往往发生电路短路。以23℃的固化前的各成分的体积为基础来决定体积％，各成分的体积，可以利用比重从重量换算成体积。另外，也可以不用在量筒中将该成分溶解或膨润，而加入很好湿润该成分的合适溶剂(水、醇等)，然后加入该成分，求出增加的体积作为其体积。 
在本发明的粘合剂组合物中，也可以适宜地添加以烷氧基硅烷衍生物或硅氨烷衍生物为代表的偶联剂和密合提高剂、流平剂等添加剂。 
本发明的粘合剂组合物，以提高交联率为目的，除了上述(b)成分外，也可以适宜地添加具有利用烯丙基、马来酰亚胺基、乙烯基等活性自由基发生聚合的官能基的化合物。具体的可举出N-乙烯咪唑、N-乙烯吡啶、N-乙烯吡咯烷酮、N-乙烯甲酰胺、N-乙烯己内酰胺、4，4′-偏乙烯双(N，N-二甲基苯胺)、N-乙烯乙酰胺、N，N-二甲基丙烯酰胺、N-异丙基丙烯酰胺、N，N-二乙基丙烯酰胺、丙烯酰胺等。 
本发明的粘合剂组合物，以提高流动性为目的，也可以并用单官能(甲基)丙烯酸酯。具体的可举出季戊四醇(甲基)丙烯酸酯、(甲基)丙烯酸-2-氰乙酯、(甲基)丙烯酸环己酯、(甲基)丙烯酸二环戊烯酯、(甲基)丙烯酸二环戊氧基乙酯、(甲基)丙烯酸-2-(2-乙氧基乙氧基)乙酯、(甲基)丙烯酸-2-乙氧基乙酯、(甲基)丙烯酸-2-乙基己酯、(甲基)丙烯酸正己酯、(甲基)丙烯酸-2-羟基乙酯、(甲基)丙烯酸羟基丙酯、(甲基)丙烯酸异冰片酯、(甲基)丙烯酸异癸酯、(甲基)丙烯酸异辛酯、(甲基)丙烯酸正月桂酯、(甲基)丙烯酸-2-甲氧基乙酯、(甲基)丙烯酸-2-苯氧基乙酯、(甲基)丙烯酸四氢呋喃酯、2-(甲基)丙烯氧基乙基磷酸酯、N，N-二甲氨基乙基(甲基)丙烯酸酯、N，N-二甲氨基丙基(甲基)丙烯酸酯、(甲基)丙烯酰基吗啉等。 
本发明的粘合剂组合物，在室温是浆状时可以原封不动的以浆状使用。在室温是固体时，除加热使用外，也可以使用溶剂使其浆化。作为能够使用的溶剂，只要是与粘合剂组合物和添加剂没有反应性、并显示充分的溶解性的溶剂，就不受特别限制，但优选在常压下的沸点是50～150℃的溶剂。在沸点是低于或等于50℃时，如果在室温放置就有挥发的危险，因而在开放体系中的使用被限制。另外，如果沸点是高于或等于150℃，使溶剂挥发困难，就有给粘合后的可靠性带来不良影响的危险。 
本发明的粘合剂组合物适合制成薄膜状使用。根据需要在粘合剂组合物中加入溶剂等形成溶液，将该溶液涂布在氟树脂薄膜、聚对苯二甲酸乙二醇酯薄膜、脱模纸等剥离性基材上，或者使上述溶液含浸在无纺布等基材中而载置在剥离性基材上，去除溶剂等就可以作为薄膜使用。如果以薄膜状使用， 从操作性等方面来看，是更方便的。 
本发明的粘合剂组合物可以利用光照射和/或加热，还可以同时一边加压一边使其粘合。通过并用这些措施，更低温短时间下的粘合成为可能。光照以150～750nm波长范围的照射光为好，最好是使用低压水银灯、中压水银灯、高压水银灯、超高压水银灯、氙灯、金属卤化灯，以0.1～10J/cm2的照射量进行固化。加热温度没有特别的限制，但以50～175℃的温度为好。压力如果是在对被粘合体没有损伤的范围内，就不受特别限制，一般以0.1～10MPa为好。这些加热和加压优选在0.5秒～3小时的范围进行。 
本发明的粘合剂组合物，例如可以作为热膨胀系数不同的不同种类的被粘合体的粘合剂使用。具体地说，可以作为以各向异性导电粘合剂、银浆、银薄膜等为代表的电路连接材料，CSP用弹性体，CSP用不充满材，以LOD胶带等为代表的半导体元件粘合材料使用。 
本发明的电路连接用粘合剂组合物由上述粘合剂组合物构成，例如，如以后所述，可以用于得到电路构件相互间被连接了的连接体或半导体装置。 
以下，一面参照附图，一面说明连接体和半导体装置的实施方式。在图的说明中，同一元件附以同一符号，省略重复的说明。另外，图中的尺寸不一定和实际的尺寸一致。 
图1是表示使用不含导电粒子的电路连接用粘合剂组合物、有关实施方式的连接体的剖面图。 
图1所示的连接体100具备：在第一电路基板31的主面31a上具有第一电路电极32的第一电路构件30，在第二电路基板41的主面41a上具有第二电路电极42的第二电路构件40，以及在第一电路电极32和第二电路电极42对置的状态下设置在第一电路构件30和第二电路构件40之间的、使第一电路电极32和第二电路电极42形成电连接的电路连接构件10C。电路连接构件10C由电路连接用粘合剂组合物10(作为该电路连接用粘合剂组合物，能够应用上述的粘合剂组合物)的固化物构成。另外第一电路电极32和第二电路电极42通过相互连接形成了电连接。 
图1所示的连接体100，例如可以像以下那样制造。 
首先，如图2所示，准备第一电路构件30、第二电路构件40和已成形 为薄膜状的电路连接用粘合剂组合物10。接着，将电路连接用粘合剂组合物10载置在第二电路构件40的形成有第二电路电极42的面上，进而，在使第一电路电极32和第二电路电极42对置的状态下，将第一电路构件30载置在电路连接用粘合剂组合物10上。接着，借助第一电路构件30和第二电路构件40，一边加热电路连接用粘合剂组合物10一边使其固化，同时在垂直于主面31a、41a的方向加压，在第一和第二电路构件30、40之间形成电路连接构件10C，得到图1的连接体100。 
图3是表示有关使用含有导电粒子的电路连接用粘合剂组合物的实施方式的连接体的剖面图。 
图3所示的连接体200具备：在第一电路基板31的主面31a上具有第一电路电极32的第一电路构件30，在第二电路基板41的主面41a上具有第二电路电极42的第二电路构件40，以及在第一电路电极32和第二电路电极42对置的状态下设置在第一电路构件30和第二电路构件40之间的、使第一电路电极32和第二电路电极42形成电连接的电路连接构件20C。电路连接构件20C是在树脂组合物21中分散了导电粒子22的电路连接用粘合剂组合物20的固化物(即，在树脂组合物的固化物21中分散了导电粒子22的固化物)，在对置的第一电路电极32和第二电路电极42之间，由于导电粒子22与两电路电极接触，借助导电粒子22而在两电路电极间形成电连接。 
图3所示的连接体200，例如可以像图4所示，准备第一电路构件30、第二电路构件40和已成形为薄膜状的电路连接用粘合剂组合物20，采用和得到上述图1的连接体100相同的方法来制造。电路连接用粘合剂组合物20是在树脂组合物21中分散了导电粒子22的组合物，可以使用上述粘合剂组合物(但是，是不含导电粒子的粘合剂组合物)作为树脂组合物21。 
作为构成电路基板的材料，可以单独使用或者组合使用半导体、玻璃、陶瓷等无机材料，聚酰亚胺、聚碳酸酯等有机材料，或由玻璃纤维/环氧树脂构成的复合材料等。 
作为具有电路电极的电路构件的具体例子，可举出液晶显示元件、卷带式封装(TCP)、2层结构软性印制电路板(FPC)等，将这些进行组合，可以作为电路电极相互间形成了电连接的连接体。 
图5是有关实施方式的半导体装置的斜视图。该半导体装置是，在半导体元件的电极和与其对置的搭载用基板(电路构件)的电极之间，将电路连接用粘合剂组合物介入，并对半导体元件的电极和与其对置的搭载用基板(电路构件)的电极加压，使加压方向的电极间形成电连接的电路连接方法中，作为电路连接用粘合剂组合物，使用上述粘合剂组合物作为电路连接用粘合剂组合物从而形成了连接的半导体装置的一例。 
图5所示的半导体装置300具备：半导体元件50、在电路基板61的主面61a上具有电路电极62的电路构件60、和在半导体元件50的连接电极和电路电极62对置的状态下设置在半导体元件50和电路构件60之间的电路连接构件20C。此时，电路电极62和半导体元件50的连接电极(在图6中作为连接电极52表示)形成了电连接。 
图6是沿图5的VI-VI线的剖面图。 
图6所示的半导体装置具备：在半导体元件本体51的主面51a上具有连接电极52的半导体元件50，在电路基板61的主面61a上具有电路电极62的电路构件60，以及在连接电极52和电路电极62对置的状态下设置在半导体元件50和电路构件60之间的、使连接电极52和电路电极62形成电连接的电路连接构件20C。在此，电路连接构件20C是在树脂组合物21中分散了导电粒子22的电路连接用粘合剂组合物20的固化物(即，在树脂组合物的固化物21C中分散了导电粒子22的固化物)，在对置的连接电极52和电路电极62之间，由于导电粒子22与两电极接触，借助导电粒子而在两电极相互间形成电连接。 
通过准备半导体元件50、电路构件60和电路连接用粘合剂组合物20，采用和得到上述图1的连接体100相同的方法，可以制造半导体装置300。 
作为半导体装置的具体例子，可举出连接了作为半导体元件的IC(集成电路)芯片和芯片连接基板的装置等。 
以下，根据实施例具体地说明本发明，但本发明不受这些实施例的限制。 
实施例1、2、对比例1 
作为(a)热塑性树脂，在60g甲基乙基酮中溶解40g苯氧基树脂(PKHC，联合ユニオンカ-バイト公司制商品名，平均分子量45000)，形成固形分为 40重量％的溶液。作为(b)自由基聚合性化合物，使用异氰脲酸EO改性二丙烯酸酯(M-215，东亚合成株式会社制商品名)和2-(甲基)丙烯酰氧基乙基磷酸酯(ライトエステルP-2M，共荣社株式会社制商品)；作为(c)固化剂，使用1，1-双(叔己基过氧)-3，3，5-三甲基环己烷(パ-ヘキサTMH，日本油脂株式会社制商品名)；作为液状橡胶，使用液状丁腈橡胶(Nipol 1312或者NipolDN601，日本ゼオン株式会社制商品名)。使用东京计器制E型粘度计EHD2557，以转子转数1r/min测定这些液状橡胶单独时在25℃的粘度时，Nipol 1312是183Pa·s，Nipol DN601是225Pa·s。另外，在以聚苯乙烯为核的粒子的表面设置厚0.2μm的镍层，在该镍层的外侧设置厚0.02μm的金层，制成平均粒径5μm、比重2.5的导电粒子。 
按固形重量比如表1所示进行配合，再配合分散1.5体积％导电粒子，然后使用涂装装置将其涂布在厚80μm的氟树脂薄膜上，然后在70℃热风干燥10分钟，得到粘合剂层的厚度是15μm的薄膜状粘合剂。 
表1 
<粘合强度、连接电阻的测定> 
使用由上述制法得到的薄膜状粘合剂，用热压接装置(加热方式：恒定加热型，东谰纪霓林格(东レエンジニアリング)株式会社制)，在160℃、以 3MPa对在38μm厚的聚酰亚胺薄膜上具有500条线宽50μm、间距100μm、厚8μm的铜电路的2层结构柔性电路板(FPC)和形成有0.2μm的ITO薄层的玻璃(厚1.1mm、表面电阻20Ω/□)进行10秒的加热加压，覆盖宽度2mm进行连接，制成连接体。在刚粘合之后和在85℃、相对湿度85％的高温高湿槽中保持120小时后，用伏-欧-毫安表测定该连接体的邻接电路间的电阻值。电阻值以邻接电路间的150个点的电阻的平均值(x+3σ；σ：标准偏差)表示。 
另外，按照JIS Z0237，使用90度剥离法测定该连接体的粘合强度，进行评价。在此，粘合强度的测定装置使用东洋博路宕(ボ-ルドウイン)株式会社制潭吸隆(テンシロン)UTM-4(剥离速度50mm/min，25℃)。如上进行的连接体的粘合强度、连接电阻的测定结果示于表2中。 
对比例2 
除使用5重量份数的在25℃是固体的丁腈橡胶(Nipol HF01，日本哉欧恩(ビオン)株式会社制商品名)代替实施例1的液状橡胶以外，其余和实施例1相同地制成薄膜状粘合剂，进行评价。此外，Nipol HF01在25℃是固体，因此仅为橡胶时的粘度测定是不可能的。 
表2 
Figure 2006101371470A00800021
实施例1、2得到的粘合剂组合物，在刚粘合后和在85℃、相对湿度85％的高温高湿槽中保持120小时后，都显示良好的连接电阻和粘合强度，同时保持高耐蚀性。与此相反，在不使用本发明中的液状橡胶的情况下(对比例1)，在刚粘合后显示了良好的值，但在85℃、相对湿度85％的高温高湿槽中保持120小时后，连接电阻上升，而且粘合强度在刚粘合后和在85℃、相对湿度85％的高温高湿槽中保持120小时后，都显示低值。另外，添加了25℃时固体状的橡胶的对比例2中，不仅连接电阻高，而且是低粘合强度，得不到满意的连接体。 
实施例3将实施例1得到的薄膜状粘合剂进行真空包装，在40℃放置5天后，同样地进行了FPC和ITO的加热压接时，发现刚粘合后的连接电阻是2.1Ω，粘合强度是760N/m，在85℃、相对湿度85％的高温高湿槽中保持120小时后的连接电阻是2.9Ω，粘合强度是700N/m，刚粘合后和可靠性试验后都显示和放置前一样的良好值，保存稳定性优良。 
实施例4 
除作为(c)固化剂使用3重量份数1，1，3，3-四甲丁基过氧-2-乙基己酸酯(パ-オクタ○，日本油脂株式会社制商品名)以外，采用和实施例1相同的方法制作薄膜状粘合剂，进行评价。其结果是，粘合强度在刚粘合后是900N/m，在85℃、相对湿度85％的高温高湿槽中保持120℃后是750N/m，连接电阻在刚粘合后显示2.3Ω，刚粘合后和可靠性试验后都显示良好的粘合强度和连接电阻。 
产业上的应用可能性 
按照本发明，能够提供以低温短时间的固化显示高粘合力、而且保存稳定性好的粘合剂组合物、电路连接用粘合剂组合物、连接体和半导体装置。 

Claims (8)

1.薄膜状电路连接用粘合剂组合物，使电路基板的主面上具有电路电极的、对置的电路构件相互间粘合，目的在于使一方的电路构件的电路电极和另一方的电路构件的电路电极形成电连接，该电路连接用粘合剂组合物含有热塑性树脂、具有2个或2个以上(甲基)丙烯酰基的自由基聚合性化合物、利用150～750nm的光照射和/或80～200℃的加热产生自由基的固化剂、平均粒径1～18μm的导电粒子、单独时在25℃的粘度是10～1000Pa·s的液状橡胶，其中，相对于电路连接用粘合剂组合物总体积，含有所述导电粒子0.1～10体积％，并且所述导电粒子是在塑料核上被覆金属、金属粒子或碳黑而成的导电粒子，或者是热熔融金属粒子。
2.根据权利要求1所述的薄膜状电路连接用粘合剂组合物，其为各向异性导电性。
3.根据权利要求1所述的薄膜状电路连接用粘合剂组合物，其中，所述液状橡胶的丙烯腈含量是10～60％。
4.根据权利要求1所述的薄膜状电路连接用粘合剂组合物，其中，所述液状橡胶是从聚异戊二烯、聚丁二烯、苯乙烯-丁二烯共聚物、丙烯腈-丁二烯共聚物、聚(氧丙烯)、聚(氧四亚甲基)二醇、聚烯烃二醇、聚-ε-己内酯及其改性物组成的组中选择的至少一种液状橡胶。
5.根据权利要求1所述的薄膜状电路连接用粘合剂组合物，其中，所述液状橡胶是从液状聚异戊二烯，液状聚丁二烯，羧基末端液状聚丁二烯，羟基末端液状聚丁二烯，液状苯乙烯-丁二烯橡胶，羟基末端液状苯乙烯-丁二烯橡胶，液状丙烯腈-丁二烯橡胶，在聚合物末端含有羧基、羟基、(甲基)丙烯酰基或者吗啉基的液状丙烯腈-丁二烯橡胶，液状羧基化丁腈橡胶，羟基末端液状聚(氧丙烯)，烷氧基甲硅烷基末端液状聚(氧丙烯)，液状聚(氧四亚甲基)二醇，液状聚烯烃二醇，液状聚-ε-己内酯组成的组中选择的至少一种液状橡胶。
6.根据权利要求1所述的薄膜状电路连接用粘合剂组合物，其中，所述液状橡胶是从液状丙烯腈-丁二烯橡胶，在聚合物末端含有羧基、羟基、(甲基)丙烯酰基或者吗啉基的液状丙烯腈-丁二烯橡胶，液状羧基化丁腈橡胶组成的组中选择的至少一种液状橡胶。
7.根据权利要求1所述的薄膜状电路连接用粘合剂组合物，其中，所述液状橡胶是从液状1，2-聚丁二烯，羧基末端液状1，2-聚丁二烯，羟基末端液状1，2-聚丁二烯组成的组中选择的至少一种液状橡胶。
8.根据权利要求1所述的薄膜状电路连接用粘合剂组合物，其中，相对于100重量份数所述热塑性树脂，含有50～250重量份数所述自由基聚合性化合物、0.5～30重量份数所述固化剂和1～50重量份数所述液状橡胶。
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