CN102449095B - 粘接剂组合物、连接结构体、连接结构体的制造方法以及粘接剂组合物的应用 - Google Patents

粘接剂组合物、连接结构体、连接结构体的制造方法以及粘接剂组合物的应用 Download PDF

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CN102449095B
CN102449095B CN201180001017.3A CN201180001017A CN102449095B CN 102449095 B CN102449095 B CN 102449095B CN 201180001017 A CN201180001017 A CN 201180001017A CN 102449095 B CN102449095 B CN 102449095B
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adhesive composite
methyl
circuit block
acid
circuit
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CN201180001017.3A
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CN102449095A (zh
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伊泽弘行
加藤木茂树
工藤直
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Resonac Corp
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Hitachi Chemical Co Ltd
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Abstract

本发明提供粘接剂组合物，其是用于连接主面上具有第一连接端子的第一电路部件和主面上具有第二连接端子的第二电路部件的粘接剂组合物，粘接剂组合物含有(a)热塑性树脂、(b)自由基聚合性化合物、(c)自由基聚合引发剂和(d)具有磷酸基的乙烯基化合物，(b)自由基聚合性化合物包含具有20～40mN/m的临界表面张力的聚氨酯(甲基)丙烯酸酯。

Description

粘接剂组合物、连接结构体、连接结构体的制造方法以及粘接剂组合物的应用
技术领域
本发明涉及粘接剂组合物、连接结构体、连接结构体的制造方法、以及粘接剂组合物的应用。
背景技术
在半导体元件和液晶显示元件中，为了使元件中的各种部件结合，一直以来使用各种粘接剂组合物。对粘接剂的要求，以粘接性为代表，广泛地涉及耐热性、高温高湿状态下的可靠性等。此外，关于粘接所使用的粘附体，可使用以印刷线路板或聚酰亚胺、聚对苯二甲酸乙二醇酯(PET)、聚碳酸酯(PC)、聚萘二甲酸乙二醇酯(PEN)等有机基材为主，铜、铝等金属或ITO(铟和锡的复合氧化物)、IZO(铟和锌的复合氧化物)、SiN、SiO2等具有各种表面状态的基材，因此需要符合各粘附体的粘接剂组合物的分子设计。此外，近年来，由于搭载半导体元件和液晶显示元件的电子设备的薄型化，因此要求作为粘附体的基材也薄型化。
一直以来，作为上述半导体元件、液晶显示元件用的粘接剂，可以使用采用了显示高粘接性且高可靠性的环氧树脂的热固性树脂(例如，参照专利文献1)。作为树脂的构成成分，一般使用环氧树脂、与环氧树脂具有反应性的酚醛树脂等固化剂、促进环氧树脂与固化剂反应的热潜伏性催化剂。热潜伏性催化剂是在室温等储存温度下不反应而在加热时显示高反应性的物质，是决定固化温度和固化速度的重要因子，从粘接剂在室温下的储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。作为实际工序中的固化条件，通过在170～250℃的温度固化1～3小时，获得了所需的粘接。
然而，随着最近的半导体元件的高集成化、液晶元件的高精细化，元件之间和线路之间间距狭小化，固化时的加热可能会对周边部件带来不良影响。而且为了低成本化，存在提高生产能力的必要性，因而要求在更低温且更短时间内固化，换言之，需要在低温快速固化条件下的粘接。为了实现该低温快速固化，需要使用活化能低的热潜伏性催化剂，但难以兼备室温附近的储存稳定性。
其中，自由基固化型粘接剂受到关注，其合并使用了丙烯酸酯衍生物、甲基丙烯酸酯衍生物等自由基聚合性化合物与作为自由基聚合引发剂的过氧化物。自由基固化型粘接剂，由于作为反应活性种的自由基富有反应性，因此可以短时间固化(例如，参照专利文献2)。然而，自由基固化型粘接剂，由于加热时的固化收缩大，因此与使用环氧树脂的情况相比，粘接强度差。针对这样的粘接强度的降低，提出了通过醚键赋予挠性、改善了粘接强度的粘接剂(参照专利文献3、4)。此外，还提出了使包含橡胶系弹性材料的应力吸收粒子分散在粘接剂中来实现粘接强度的改善的粘接剂(参照专利文献5)。
专利文献1：日本特开平1-113480号公报
专利文献2：日本特开2002-203427号公报
专利文献3：日本特许第3522634号公报
专利文献4：日本特开2002-285128号公报
专利文献5：日本特许第3477367号公报
发明内容
发明所要解决的课题
然而，由于自由基固化型粘接剂在低温、短时间内固化，因此对聚酰亚胺、PET、PC、PEN等有机基材、ITO、IZO、SiN、SiO2等无机基材的润湿性难以充分地获得。例如，即使使用上述专利文献3～5中记载的方法，也会产生得不到对上述有机基材、无机基材的充分的润湿性、粘接强度降低的问题。此外，随着作为粘附体的上述有机基材、无机基材的薄型化，更加需要粘接剂组合物的挠性化、伸长，但在上述专利文献3、4记载的方法中，存在粘接剂组合物得不到充分的挠性、伸长，粘接强度降低的问题。
因此，本发明的目的是提供即使在低温、短时间的固化条件下也可以获得优异的粘接强度、并即使在长时间的可靠性试验(高温高湿试验)之后也可以保持稳定的性能(粘接强度、连接电阻)的粘接剂组合物、使用了该粘接剂组合物的电路部件的连接结构体、连接结构体的制造方法、以及粘接剂组合物的应用。
解决课题的实施方案
为了达到上述目的，本发明提供一种粘接剂组合物(第1粘接剂组合物)，其是用于连接主面上具有第一连接端子的第一电路部件和主面上具有第二连接端子的第二电路部件的粘接剂组合物，粘接剂组合物含有(a)热塑性树脂、(b)自由基聚合性化合物、(c)自由基聚合引发剂和(d)具有磷酸基的乙烯基化合物，(b)自由基聚合性化合物包含具有20～40mN/m的临界表面张力的聚氨酯(甲基)丙烯酸酯。
上述第1粘接剂组合物含有上述各成分，并且(b)自由基聚合性化合物包含具有20～40mN/m的临界表面张力的聚氨酯(甲基)丙烯酸酯，由此可以提高对聚酰亚胺、PET、PC、PEN等有机基材、ITO、IZO、SiN、SiO2等无机基材的润湿性，可以实现低温固化条件下的粘接，可以提高电路部件之间的粘接强度。此外，即使在长时间的可靠性试验之后也可以保持稳定的性能。
本发明的第1粘接剂组合物，优选聚氨酯(甲基)丙烯酸酯在25℃的粘度为600～5000Pa·s。通过使聚氨酯(甲基)丙烯酸酯在25℃的粘度在上述范围内，可以获得适度的流动性，提高润湿性，提高电路部件之间的粘接强度。
此外，本发明的第1粘接剂组合物，优选聚氨酯(甲基)丙烯酸酯的重均分子量为10000以上且小于25000。通过使聚氨酯(甲基)丙烯酸酯的重均分子量在上述范围内，可以赋予粘接剂组合物以适度的挠性，提高电路部件之间的粘接强度，获得优异的连接可靠性。
本发明的第1粘接剂组合物，优选断裂伸长率为300～500％。通过使断裂伸长率在上述范围内，可以赋予粘接剂组合物以充分的挠性，提高电路部件之间的粘接强度，获得优异的连接可靠性。
本发明提供一种粘接剂组合物(第2粘接剂组合物)，其是用于连接主面上具有第一连接端子的第一电路部件和主面上具有第二连接端子的第二电路部件的粘接剂组合物，粘接剂组合物含有(a)热塑性树脂、(b)自由基聚合性化合物和(c)自由基聚合引发剂，(b)自由基聚合性化合物包含聚氨酯(甲基)丙烯酸酯，断裂伸长率为300～500％。
上述第2粘接剂组合物含有上述各成分，并且(b)自由基聚合性化合物包含聚氨酯(甲基)丙烯酸酯，断裂伸长率在上述范围内，由此可以赋予充分的挠性，追随粘附体(聚酰亚胺、PET、PC、PEN等)的变形，因此可以提高电路部件之间的粘接强度，获得优异的连接可靠性。
本发明的第2粘接剂组合物，优选还含有(d)具有磷酸基的乙烯基化合物。通过含有(d)具有磷酸基的乙烯基化合物，可以提高对金属基材的粘接性。此外，可以获得对具有由金属或ITO、IZO等构成的连接端子的电路部件的优异的粘接强度。
本发明的第1和/或第2粘接剂组合物，优选在200℃时的储能模量为0.5～5MPa。认为通过使在200℃时的储能模量在上述范围内，可以兼有充分的挠性和交联密度，并缓和了粘接剂组合物的粘附体与粘接剂组合物界面的应力。因此，可以提高电路部件之间的粘接强度，并且即使在长时间的可靠性试验之后也可以保持稳定的性能。
此外，本发明的第1和/或第2粘接剂组合物，优选(a)热塑性树脂含有选自苯氧树脂、聚氨酯树脂、聚酯型聚氨酯树脂、丁醛树脂、丙烯酸树脂和聚酰亚胺树脂组成的组中的至少1种树脂。作为(a)热塑性树脂，含有上述树脂，由此可进一步提高粘接剂组合物的耐热性、粘接性。
此外，本发明的第1和/或第2粘接剂组合物，优选还含有(e)导电性粒子。通过含有(e)导电性粒子，可以赋予粘接剂组合物以良好的导电性或各向异性导电性，因此可以更适合用于具有连接端子的电路部件彼此之间的粘接用途等。此外，可以更充分地降低介由上述第1和/或第2粘接剂组合物而进行了电连接的电路部件的连接电阻。
此外，本发明提供一种电路部件的连接结构体，包括：主面上具有第一连接端子的第一电路部件、主面上具有第二连接端子的第二电路部件、和连接部件，以第一连接端子和第二连接端子相对的方式，将第一电路部件和第二电路部件介由包含上述第1和/或第2粘接剂组合物的连接部件而配置，并且第一连接端子和第二连接端子被电连接，第一电路部件和/或第二电路部件由包含玻璃化转变温度为200℃以下的热塑性树脂的基材构成。
这样的连接结构体，由于一对电路部件的连接可使用本发明的上述第1和/或第2粘接剂组合物的固化物，因此可以追随包含玻璃化转变温度为200℃以下的热塑性树脂的基材的变形，也可以提高对基材的润湿性，充分地提高电路部件之间的粘接强度。此外，即使在长时间的可靠性试验之后也可以保持稳定的性能。
在本发明的电路部件的连接结构体中，玻璃化转变温度为200℃以下的热塑性树脂优选为选自聚对苯二甲酸乙二醇酯、聚碳酸酯和聚萘二甲酸乙二醇酯中的至少1种树脂。上述连接结构体，由于一对电路部件的连接可使用本发明的上述第1和/或第2粘接剂组合物的固化物，因此可以追随包含聚对苯二甲酸乙二醇酯等基材的变形，也可以提高对基材的润湿性，充分地提高电路部件之间的粘接强度。此外，即使在长时间的可靠性试验之后也可以保持稳定的性能。
此外，在本发明的电路部件的连接结构体中，第一电路部件或第二电路部件中的一个电路部件由含有选自聚对苯二甲酸乙二醇酯、聚碳酸酯和聚萘二甲酸乙二醇酯组成的组中的至少1种材料的基材构成，第一电路部件或第二电路部件中的另一电路部件优选是聚酰亚胺树脂。本连接结构体中，第一电路部件和第二电路部件用上述那样的基材来构成，由此可以进一步提高与粘接剂组合物的润湿性和粘接强度，获得优异的连接可靠性。
本发明提供一种电路部件的连接结构体的制造方法，包括下述工序：将主面上具有第一连接端子的第一电路部件和主面上具有第二连接端子的第二电路部件介由上述粘接剂组合物以第一连接端子和第二连接端子相对的方式配置的工序；以及将粘接剂组合物加热、使其固化，从而连接第一电路部件和第二电路部件的工序。根据本制造方法，通过将第一电路部件和第二电路部件用上述粘接剂组合物连接，可以获得具有优异的连接可靠性的电路部件的连接结构体。
此外，本发明提供一种粘接剂组合物的应用，用于连接主面上具有第一连接端子的第一电路部件和主面上具有第二连接端子的第二电路部件，所述粘接剂组合物(第1粘接剂组合物)含有(a)热塑性树脂、(b)自由基聚合性化合物、(c)自由基聚合引发剂和(d)具有磷酸基的乙烯基化合物，(b)自由基聚合性化合物包含具有20～40mN/m的临界表面张力的聚氨酯(甲基)丙烯酸酯。上述第1粘接剂组合物，由于含有上述各成分，并且(b)自由基聚合性化合物包含具有20～40mN/m的临界表面张力的聚氨酯(甲基)丙烯酸酯，因此可以提高对聚酰亚胺、PET、PC、PEN等有机基材、ITO、IZO、SiN、SiO2等无机基材的润湿性，可以实现低温固化条件下的粘接，可以提高电路部件之间的粘接强度。此外，即使在长时间的可靠性试验之后也可以保持稳定的性能。
在上述应用中，优选聚氨酯(甲基)丙烯酸酯在25℃时的粘度为600～5000Pa·s。通过使聚氨酯(甲基)丙烯酸酯在25℃时的粘度在上述范围内，可以获得适度的流动性，提高润湿性，获得优异的连接可靠性。
在上述应用中，优选聚氨酯(甲基)丙烯酸酯的重均分子量为10000以上且小于25000。通过使聚氨酯(甲基)丙烯酸酯的重均分子量在上述范围内，可以赋予粘接剂组合物以适度的挠性，提高电路部件之间的粘接强度，获得优异的连接可靠性。
在上述应用中，优选粘接剂组合物的断裂伸长率为300～500％。通过使断裂伸长率在上述范围内，可以赋予粘接剂组合物以充分的挠性，提高电路部件之间的粘接强度，获得优异的连接可靠性。
此外，本发明提供一种粘接剂组合物的应用，用于连接主面上具有第一连接端子的第一电路部件和主面上具有第二连接端子的第二电路部件，所述粘接剂组合物(第2粘接剂组合物)含有(a)热塑性树脂、(b)自由基聚合性化合物和(c)自由基聚合引发剂，(b)自由基聚合性化合物包含聚氨酯(甲基)丙烯酸酯，断裂伸长率为300～500％。上述第2粘接剂组合物，由于含有上述各成分，并且(b)自由基聚合性化合物包含聚氨酯(甲基)丙烯酸酯，断裂伸长率在上述范围内，从而可以赋予充分的挠性，并追随粘附体(聚酰亚胺、PET、PC、PEN等)的变形，因此可以提高电路部件之间的粘接强度，获得优异的连接可靠性。
在上述应用中，粘接剂组合物优选还含有(d)具有磷酸基的乙烯基化合物。通过含有(d)具有磷酸基的乙烯基化合物，可以提高对金属基材的粘接性，而且还可以获得对具有由金属、ITO、IZO等构成的连接端子的电路部件的优异的粘接强度。
在上述应用中，优选粘接剂组合物在200℃时的储能模量为0.5～5MPa。认为通过使在200℃的储能模量在上述范围内，可以兼有充分的挠性和交联密度，缓和了粘接剂组合物的粘附体与粘接剂组合物界面的应力。因此，可以提高电路部件之间的粘接强度，并且即使在长时间的可靠性试验之后也可以保持稳定的性能。
在上述应用中，优选(a)热塑性树脂含有选自苯氧树脂、聚氨酯树脂、聚酯型聚氨酯树脂、丁醛树脂、丙烯酸树脂和聚酰亚胺树脂组成的组中的至少1种树脂。作为(a)热塑性树脂，通过含有上述树脂，可进一步提高粘接剂组合物的耐热性、粘接性。
在上述应用中，优选粘接剂组合物还含有(e)导电性粒子。通过含有(e)导电性粒子，可以赋予粘接剂组合物以良好的导电性或各向异性导电性，从而可以更适合用于具有连接端子的电路部件彼此之间的粘接用途等，并可以更充分地降低介由上述第1和/或第2粘接剂组合物而进行了电连接的电路部件的连接电阻。
发明效果
根据本发明，可以提供即使在低温的固化条件下也可以获得优异的粘接强度、并即使在长时间的可靠性试验(高温高湿试验)之后也可以保持稳定的性能(粘接强度、连接电阻)的粘接剂组合物、使用了该粘接剂组合物的电路部件的连接结构体、连接结构体的制造方法、以及粘接剂组合物的应用。
附图说明
图1是显示使用了本发明的粘接剂组合物的电路部件的连接结构体的一个实施方式的剖面示意图。
图2是显示在制作图1所示的电路部件的连接结构体之前的第一电路部件、第二电路部件和粘接剂组合物的剖面示意图。
图3是显示使用了本发明的粘接剂组合物(含有导电性粒子)的电路部件的连接结构体的一个实施方式的剖面示意图。
图4是显示在制作图3所示的电路部件的连接结构体之前的第一电路部件、第二电路部件和粘接剂组合物(含有导电性粒子)的剖面示意图。
具体实施方式
以下，根据情况参照附图对本发明的优选实施方式进行详细说明。另外，在附图中，对相同或相应部分标记相同符号，省略重复的说明。此外，在本发明中，(甲基)丙烯酸表示丙烯酸或与其对应的甲基丙烯酸，(甲基)丙烯酸酯是指丙烯酸酯或与其对应的甲基丙烯酸酯，(甲基)丙烯酰基是指丙烯酰基或甲基丙烯酰基。
本实施方式中的“临界表面张力(γc)”是指，使液体的聚氨酯(甲基)丙烯酸酯或聚氨酯(甲基)丙烯酸酯溶解在溶剂中，将所得的液体物通过涂覆装置涂布在氟树脂膜上，在70℃、10分钟或可以除去所使用的溶剂的温度和时间下进行热风干燥，实际测定在23℃分别向所得的膜状的聚氨酯(甲基)丙烯酸酯滴加纯水、润湿张力试验用混合溶液No.50、60(和光纯药工业(株)制)1μl之后即刻的与聚氨酯(甲基)丙烯酸酯表面所成的角(接触角θ)，当将各液体的表面张力设为x轴、将COSθ设为y轴绘图时，直线在Y＝1时的表面张力。另外，在穿过由上述纯水、No.50、60测定所得的3点的直线在Y＝1时、在X变为负值的情况下，也可以使用纯水、润湿张力试验用混合溶液No.60、1-溴萘(和光纯药工业(株)制)进行与上述同样的测定，使用穿过所得的3点的直线当Y＝1时的表面张力的值。
此外，本实施方式中的“储能模量”是指，将粘接剂组合物通过涂覆装置涂布在氟树脂膜上，在70℃、10分钟或可以除去所使用的溶剂的温度和时间下进行热风干燥，将所得的膜状的粘接剂组合物在180℃加热固化1小时，将所得的样品使用TA仪器公司制粘弹性分析器“RSA-3”(商品名)，在升温速度5℃/分钟、频率10Hz、测定温度-150～300℃的条件下测定，在200℃的储能模量(E’)的值。
本实施方式中的“断裂伸长率”是指，将粘接剂组合物通过涂覆装置涂布在氟树脂膜上，在70℃、10分钟或可以除去所使用的溶剂的温度和条件下进行热风干燥，将所得的膜状的粘接剂组合物在180℃加热固化1小时，将所得的样品使用英斯特朗公司制材料试验机“microtester5548”(商品名)，在拉伸速度50mm/分钟、测定温度在25℃的条件下测定，当膜断裂时，由标点间的长度L和原来标点间距离L0使用下述式(1)计算所得的值。
断裂伸长率(％)＝(L-L0)/L0×100(1)
此外，本实施方式中的“粘度”是指将聚氨酯(甲基)丙烯酸酯使用安东帕公司制流变仪“PhysicaMCR301”(商品名)，在频率1Hz、测定温度25℃的条件下测定所得的值。
本实施方式中的“玻璃化转变温度(Tg)”是指将膜状的有机基材使用TA仪器公司制粘弹性分析器“RSA-3”(商品名)，在升温速度5℃/分钟、频率10Hz、测定温度-150～300℃的条件下测定得到的、Tg附近的tanδ峰温度的值。
此外，在本实施方式中，“重均分子量”和“数均分子量”是指按照表1所示的条件，通过凝胶渗透色谱(GPC)使用标准聚苯乙烯的标准曲线测定所得的值。
[表1]
(第1实施方式)
本发明的第1实施方式涉及的粘接剂组合物的特征在于，其是用于连接主面上具有第一连接端子的第一电路部件和主面上具有第二连接端子的第二电路部件的粘接剂组合物，粘接剂组合物含有(a)热塑性树脂、(b)自由基聚合性化合物、(c)自由基聚合引发剂、和(d)具有磷酸基的乙烯基化合物，(b)自由基聚合性化合物包含具有20～40mN/m的临界表面张力的氨基甲酸酯(甲基)丙烯酸酯。
以下，详细地说明各成分。本实施方式所使用的(a)热塑性树脂是指具有如下性质的树脂(高分子)：通过加热而变成粘度高的液体状态，通过外力而自由地变形，如果冷却并除去外力则在保持其形状的状态下变硬并可重复进行该过程。此外，也包括具有上述性质的含反应性官能团的树脂(高分子)。(a)热塑性树脂的玻璃化转变温度(Tg)优选为0～190℃，更优选为20～170℃。
作为这样的(a)热塑性树脂，可以使用聚酰亚胺树脂、聚酰胺树脂、苯氧树脂、(甲基)丙烯酸树脂、聚氨酯树脂、聚酯型聚氨酯树脂、聚乙烯醇缩丁醛树脂等。这些树脂可以单独使用或2种以上混合使用。此外，在这些热塑性树脂中可以包含硅氧烷键、氟取代基。只要是所混合的树脂彼此完全地相容、或产生微相分离而白浊的状态，就可以适合使用。
在使粘接剂组合物形成膜状而利用的情况下，上述热塑性树脂的分子量越大，越容易获得良好的膜形成性，此外，可以宽范围地设定影响作为膜状粘接剂组合物的流动性的熔融粘度。作为(a)热塑性树脂的重均分子量，优选为5,000～150,000，更优选为10,000～80,000。如果重均分子量低于5,000，则倾向于不易获得良好的膜形成性，如果大于150,000，则倾向于不易获得与其它成分的良好相容性。
粘接剂组合物中的(a)热塑性树脂的含量，以粘接剂组合物总量为基准，优选为5～80质量％，更优选为15～70质量％。如果其含量低于5质量％，则在使粘接剂组合物形成膜状而利用的情况下，特别地倾向于不易获得良好的膜形成性，如果大于80质量％，则倾向于不易获得良好的粘接剂组合物的流动性。
本实施方式的粘接剂组合物所含有的(b)自由基聚合性化合物，是指在自由基聚合引发剂的作用下发生自由基聚合的化合物，但也可以是通过赋予光、热等活化能使其本身产生自由基的化合物。作为(b)自由基聚合性化合物，可以适合使用具有例如乙烯基、(甲基)丙烯酰基、烯丙基、马来酰亚胺基等通过活性自由基来聚合的官能团的化合物。
作为(b)自由基聚合性化合物，具体而言，可列举环氧(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、三羟甲基丙烷三(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、二环戊烯基(甲基)丙烯酸酯、二环戊烯基氧基乙基(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、双苯氧基乙醇芴丙烯酸酯、使双酚芴二缩水甘油基醚的缩水甘油基与(甲基)丙烯酸加成而得的环氧(甲基)丙烯酸酯、双苯氧基乙醇芴丙烯酸酯、使双酚芴二缩水甘油基醚的缩水甘油基与(甲基)丙烯酸加成而得的环氧(甲基)丙烯酸酯、在使双酚芴二缩水甘油基醚的缩水甘油基与乙二醇和/或丙二醇加成而得的化合物中导入(甲基)丙烯酰氧基所得的化合物、下述通式(A)和(B)所示的化合物等。
[化1]
[式(A)中，R1和R2各自独立地表示氢原子或甲基，a和b各自独立地表示1～8的整数。]
[化2]
[式(B)中，R3和R4各自独立地表示氢原子或甲基，c和d各自独立地表示0～8的整数。]
此外，作为(b)自由基聚合性化合物，可以是单独在30℃下静置的情况下为蜡状(ワツクス状)、蜡质状(ろう状)、结晶状、玻璃状、粉状等无流动性、显示固体状态的化合物，可以没有特别限制地使用。作为这样的(b)自由基聚合性化合物，具体而言，可列举N，N’-亚甲基双丙烯酰胺、双丙酮丙烯酰胺、N-羟基甲基丙烯酰胺、N-苯基甲基丙烯酰胺、2-丙烯酰胺-2-甲基丙烷磺酸、三(2-丙烯酰氧基乙基)异氰脲酸酯、N-苯基马来酰亚胺、N-(邻甲基苯基)马来酰亚胺、N-(间甲基苯基)马来酰亚胺、N-(对甲基苯基)-马来酰亚胺、N-(邻甲氧基苯基)马来酰亚胺、N-(间甲氧基苯基)马来酰亚胺、N-(对甲氧基苯基)-马来酰亚胺、N-甲基马来酰亚胺、N-乙基马来酰亚胺、N-辛基马来酰亚胺、4，4’-二苯基甲烷双马来酰亚胺、间亚苯基双马来酰亚胺、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、N-甲基丙烯酰氧基马来酰亚胺、N-丙烯酰氧基马来酰亚胺、1，6-双马来酰亚胺-(2，2，4-三甲基)己烷、N-甲基丙烯酰氧基琥珀酸酰亚胺、N-丙烯酰氧基琥珀酸酰亚胺、2-萘基甲基丙烯酸酯、2-萘基丙烯酸酯、季戊四醇四丙烯酸酯、二乙烯基亚乙基脲、二乙烯基亚丙基脲、2-聚苯乙烯基乙基(甲基丙烯酸酯)、N-苯基-N’-(3-甲基丙烯酰氧基-2-羟基丙基)-对苯二胺、N-苯基-N’-(3-丙烯酰氧基-2-羟基丙基)-对苯二胺、四甲基哌啶基(甲基丙烯酸酯)、四甲基哌啶基丙烯酸酯、五甲基哌啶基(甲基丙烯酸酯)、五甲基哌啶基丙烯酸酯、十八烷基丙烯酸酯、N-叔丁基丙烯酰胺、二丙酮丙烯酰胺、N-(羟基甲基)丙烯酰胺、下述通式(C)～(L)所示的化合物等。
[化3]
[式(C)中，e表示1～10的整数。]
[化4]
[化5]
[式(E)中，R5和R6各自独立地表示氢原子或甲基，f表示15～30的整数。]
[化6]
[式(F)中，R7和R8各自独立地表示氢原子或甲基，g表示15～30的整数。]
[化7]
[式(G)中，R9表示氢原子或甲基。]
[化8]
[式(H)中，R10表示氢原子或甲基，h表示1～10的整数。]
[化9]
[式(I)中，R11表示氢原子或下述通式(i)或(ii)所示的有机基团，i表示1～10的整数。]
[化10]
[化11]
[化12]
[式(J)中，R12表示氢原子或下述通式(iii)或(iv)所示的有机基团，j表示1～10的整数。]
[化13]
[化14]
[化15]
[式(K)中，R13表示氢原子或甲基。]
[化16]
[式(L)中，R14表示氢原子或甲基。]
此外，可以将作为属于(b)自由基聚合性化合物的化合物的选自N-乙烯基化合物和N，N-二烷基乙烯基化合物中的N-乙烯基系化合物与除此以外的(b)自由基聚合性化合物合并使用。通过合并使用N-乙烯基系化合物，可以提高粘接剂组合物的交联率。
作为N-乙烯基系化合物，具体而言，可列举N-乙烯基咪唑、N-乙烯基吡啶、N-乙烯基吡咯烷酮、N-乙烯基甲酰胺、N-乙烯基己内酰胺、4，4’-亚乙烯基双(N，N-二甲基苯胺)、N-乙烯基乙酰胺、N，N-二甲基丙烯酰胺、N，N-二乙基丙烯酰胺等。
另外，后述的(d)具有磷酸基的乙烯基化合物是作为自由基聚合性化合物起作用的化合物，但本说明书中的(b)自由基聚合性化合物是指除了(d)具有磷酸基的乙烯基化合物以外的自由基聚合性化合物。
粘接剂组合物中的(b)自由基聚合性化合物的含量，相对于(a)热塑性树脂100质量份，优选为50～250质量份，更优选为60～150质量份。如果上述含量低于50质量份，则倾向于固化后不易获得充分的耐热性，此外，如果超过250质量份，则在作为膜使用的情况下，倾向于不易获得良好的膜形成性。
本实施方式的粘接剂组合物含有临界表面张力为20～40mN/m的聚氨酯(甲基)丙烯酸酯作为(b)自由基聚合性化合物。其中，在本实施方式中，更优选使用上述临界表面张力的聚氨酯丙烯酸酯。上述聚氨酯(甲基)丙烯酸酯可以通过脂肪族系二异氰酸酯和脂肪族二醇的缩合反应来获得。
构成上述聚氨酯(甲基)丙烯酸酯的脂肪族系二异氰酸酯选自丁二异氰酸酯、己二异氰酸酯、赖氨酸二异氰酸酯、2-甲基戊烷-1，5-二异氰酸酯、3-甲基戊烷-1，5-二异氰酸酯、2，2，4-三甲基六亚甲基-1，6-二异氰酸酯、2，4，4-三甲基六亚甲基-1，6-二异氰酸酯、异佛尔酮二异氰酸酯、环己基二异氰酸酯、氢化苯二亚甲基二异氰酸酯、氢化二苯基甲烷二异氰酸酯、氢化三甲基苯二亚甲基二异氰酸酯等。
此外，构成上述聚氨酯(甲基)丙烯酸酯的脂肪族二醇选自将乙二醇、丙二醇、1，2-丙二醇、1，3-丙二醇、1，3-丁二醇、1，4-丁二醇、新戊二醇、1，2-戊二醇、1，4-戊二醇、1，5-戊二醇、2，4-戊二醇、2-甲基-2，4-戊二醇、2，4-二甲基-2，4-戊二醇、2，2，4-三甲基-1，3-戊二醇、1，2-己二醇、1，5-己二醇、1，6-己二醇、2，5-己二醇、2-乙基-1，3-己二醇、2，5-二甲基-2，5-己二醇、1，2-辛二醇、1，8-辛二醇、1，7-庚二醇、1，9-壬二醇、1，2-癸二醇、1，10-癸二醇、1，12-癸二醇、十二烷二醇、频哪醇、1，4-丁炔二醇、三乙二醇、二甘醇、双丙甘醇、环己烷二甲醇等饱和的低分子二醇类，由至少1种以上的上述二醇类与碳酰氯反应所得的聚碳酸酯二醇类，以至少1种以上的上述二醇类作为引发剂将环氧乙烷、环氧丙烷、表氯醇等单体的1种或1种以上通过公知的方法加聚所得的聚醚二醇类，与己二酸、3-甲基己二酸、2，2，5，5-四甲基己二酸、马来酸、富马酸、琥珀酸、2，2-二甲基琥珀酸、2-乙基-2-甲基琥珀酸、2，3-二甲基琥珀酸、草酸、丙二酸、甲基丙二酸、乙基丙二酸、丁基丙二酸、二甲基丙二酸、戊二酸、2-甲基戊二酸、3-甲基戊二酸、2，2-二甲基戊二酸、3，3-二甲基戊二酸、2，4-二甲基戊二酸、庚二酸、辛二酸、壬二酸、癸二酸等二元酸或与它们对应的酸酐脱水缩合所得的聚酯二醇类；将ε-己内酯等环状酯化合物开环聚合所得的聚酯二醇类。由上述二醇类和二羧酸获得的聚酯二醇类既可以单独使用，也可以将2种以上聚酯二醇类混合使用。如果使用这些聚酯二醇类，则易于将聚氨酯(甲基)丙烯酸酯的临界表面张力控制在20～40mN/m的范围内。
上述聚氨酯(甲基)丙烯酸酯的临界表面张力为20～40mN/m，优选为20～35mN/m，更优选为20～33mN/m。在聚氨酯(甲基)丙烯酸酯的临界表面张力在上述范围内的情况下，与作为粘附体的聚酰亚胺、PET等临界表面张力接近，润湿性提高，因此可以提高粘接强度，获得优异的连接可靠性。此外，如果该临界表面张力低于20mN/m或超过40mN/m，则可能对聚酰亚胺、PET、PC、PEN等的润湿性降低、相容性变差。认为上述聚氨酯(甲基)丙烯酸酯的临界表面张力与氨酯键当量相关，并可以通过改变二醇的数均分子量来调整。例如，如果使二醇的数均分子量增大，则倾向于氨酯键当量减少，临界表面张力降低。
在本实施方式的粘接剂组合物中，从提高对聚酰亚胺、PET、PC、PEN等基材的粘接强度的观点出发，上述聚氨酯(甲基)丙烯酸酯的重均分子量优选在10000以上且小于25000的范围内。只要上述聚氨酯(甲基)丙烯酸酯的重均分子量在上述范围内，就可以获得柔软性和凝聚力，并可以提高与聚酰亚胺、PET、PC、PEN等有机基材的粘接强度，获得优异的连接可靠性。此外，从充分地获得上述效果的观点出发，上述聚氨酯(甲基)丙烯酸酯的重均分子量更优选为12000以上且低于20000。上述聚氨酯(甲基)丙烯酸酯的重均分子量，如果低于10000，则倾向于得不到充分的挠性，如果为25000以上，则粘接剂组合物的流动性倾向于降低。
上述聚氨酯(甲基)丙烯酸酯在25℃时的粘度优选为600～5000Pa·s，更优选为600～4500Pa·s。聚氨酯(甲基)丙烯酸酯在25℃时的粘度在上述范围内的情况下，可以获得充分的流动性，获得优异的连接可靠性。此外，可以获得适度的粘接力，操作性优异。另一方面，在低于600Pa·s的情况下，倾向于粘接力增加，操作性变差，如果超过5000Pa·s，则倾向于得不到充分的流动性，对粘附体的润湿性降低，粘接强度和连接可靠性变差。
此外，上述聚氨酯(甲基)丙烯酸酯的含量以粘接剂组合物总量为基准，优选为5～95质量％，更优选为10～80质量％。在含量低于5质量％的情况下，耐热性倾向于易于降低，如果超过95质量％，则在作为膜使用的情况下，膜形成性倾向于易于降低。
作为本实施方式的粘接剂组合物所含有的(c)自由基聚合引发剂，可以使用一直以来已知的有机过氧化物、偶氮化合物等通过从外部提供能量而产生自由基的化合物。作为(c)自由基聚合引发剂，从稳定性、反应性、相容性的观点出发，优选1分钟半衰期温度为90～175℃且分子量为180～1000的有机过氧化物。1分钟半衰期温度在该范围内，由此储存稳定性优异，充分地提高自由基聚合性，可以在短时间内固化。
作为(c)自由基聚合引发剂，具体而言，可列举1，1，3，3-四甲基丁基过氧化新癸酸酯、二(4-叔丁基环己基)过氧化二碳酸酯、二(2-乙基己基)过氧化二碳酸酯、枯基过氧化新癸酸酯、1，1，3，3-四甲基丁基过氧化新癸酸酯、过氧化二月桂酰、1-环己基-1-甲基乙基过氧化新癸酸酯、叔己基过氧化新癸酸酯、叔丁基过氧化新癸酸酯、叔丁基过氧化新戊酸酯、1，1，3，3-四甲基丁基过氧化-2-乙基己酸酯、2，5-二甲基-2，5-二(2-乙基己酰过氧化)己烷、叔己基过氧化-2-乙基己酸酯、叔丁基过氧化-2-乙基己酸酯、叔丁基过氧化新庚酸酯、叔戊基过氧化-2-乙基己酸酯、二叔丁基过氧化六氢对苯二甲酸酯、叔戊基过氧化-3，5，5-三甲基己酸酯、3-羟基-1，1-二甲基丁基过氧化新癸酸酯、1，1，3，3-四甲基丁基过氧化-2-乙基己酸酯、叔戊基过氧化新癸酸酯、叔戊基过氧化-2-乙基己酸酯、过氧化二(3-甲基苯甲酰)、过氧化二苯甲酰、过氧化二(4-甲基苯甲酰)、叔己基过氧化异丙基单碳酸酯、叔丁基过氧化马来酸酯、叔丁基过氧化-3，5，5-三甲基己酸酯、叔丁基过氧化月桂酸酯、2，5-二甲基-2，5-二(3-甲基苯甲酰过氧化)己烷、叔丁基过氧化-2-乙基己基单碳酸酯、叔己基过氧化苯甲酸酯、2，5-二甲基-2，5-二(苯甲酰过氧化)己烷、叔丁基过氧化苯甲酸酯、二丁基过氧化三甲基己二酸酯、叔戊基过氧化正辛酸酯、叔戊基过氧化异壬烯酸酯、叔戊基过氧化苯甲酸酯等有机过氧化物；2，2’-偶氮双-2，4-二甲基戊腈、1，1’-偶氮双(1-乙酰氧基-1-苯基乙烷)、2，2’-偶氮二异丁腈、2，2’-偶氮双(2-甲基丁腈)、二甲基-2，2’-偶氮二异丁腈、4，4’-偶氮双(4-氰基戊酸)、1，1’-偶氮双(1-环己烷甲腈)等偶氮化合物等。
这些化合物既可以单独使用，也可以2种以上化合物混合使用。
此外，作为(c)自由基聚合引发剂，可以使用通过150～750nm的光照射而产生自由基的化合物。作为这样的化合物，例如，Photoinitiation，Photopolymerization，andPhotocuring(光引发、光聚合和光固化)，J.-P.Fouassier，HanserPublishers(1995年，p17～p35)中所记载的α-对乙酰氨基酚衍生物、氧化膦衍生物对光照射的灵敏度高，因此更优选。
这些化合物既可以单独使用，也可以与上述有机过氧化物、偶氮化合物混合使用。
上述(c)自由基聚合引发剂的含量相对于(a)热塑性树脂100质量份优选为0.1～500质量份，更优选为1～300质量份，进一步优选为5～50质量份，特别优选为10～30质量份。如果(c)自由基聚合引发剂的含量低于0.1质量份，则粘接剂组合物倾向于不易充分地固化，如果超过500质量份，则储存稳定性倾向于变差。
作为本实施方式中的(d)具有磷酸基的乙烯基化合物(含有磷酸基的乙烯基化合物)，只要是具有磷酸基和乙烯基的化合物即可，没有特别地限制，更优选分子内具有至少一个以上自由基聚合性优异的(甲基)丙烯酰基作为乙烯基的磷酸(甲基)丙烯酸酯化合物。作为这样的化合物，可列举下述通式(M)～(O)所示的化合物。
[化17]
[式(M)中，R15表示(甲基)丙烯酰氧基，R16表示氢原子或甲基，k和l各自独立地表示1～8的整数。另外，式中，R15彼此之间、R16彼此之间、k彼此之间和l彼此之间相同或不同。]
[化18]
[式(N)中，R17表示(甲基)丙烯酰氧基，m和n各自独立地表示1～8的整数。另外，式中，R17彼此之间、m彼此之间和n彼此之间相同或不同。]
[化19]
[式(O)中，R18表示(甲基)丙烯酰氧基，R19表示氢原子或甲基，o和p各自独立地表示1～8的整数。另外，式中，R19彼此之间和o彼此之间相同或不同。]
作为(d)含有磷酸基的乙烯基化合物，具体而言，可列举酸式磷酸基氧基乙基(甲基丙烯酸酯)(acidphosphoroxyethylmethacrylate)、酸式磷酸基氧基乙基丙烯酸酯、酸式磷酸基氧基丙基(甲基丙烯酸酯)、酸式磷酸基氧基聚氧乙二醇单甲基丙烯酸酯、酸式磷酸基氧基聚氧丙二醇单甲基丙烯酸酯、2，2’-二(甲基)丙烯酰氧基二乙基磷酸酯、EO改性磷酸二(甲基丙烯酸酯)、磷酸改性环氧丙烯酸酯、磷酸乙烯酯等。
粘接剂组合物中的(d)含有磷酸基的乙烯基化合物的含量，与除了含有磷酸基的乙烯基化合物以外的(b)自由基聚合性化合物的含量独立地，相对于(a)热塑性树脂100质量份，优选为0.2～300质量份，更优选为1～200质量份，进一步优选为1～50质量份，特别优选为1～10质量份。如果(d)含有磷酸基的乙烯基化合物的含量低于0.2质量份，则倾向于不易获得高粘接强度，如果超过300质量份，则固化后的粘接剂组合物的物性倾向于容易降低，不易确保可靠性。
本实施方式的粘接剂组合物所含有的(e)导电性粒子只要是其整体或表面具有导电性的粒子即可，但在具有连接端子的电路部件的连接中使用的情况下，优选平均粒径小于连接端子间距离。
作为(e)导电性粒子，可列举Au、Ag、Ni、Cu、焊料等的金属粒子，碳等。另外，也可以是将非导电性的玻璃、陶瓷、塑料等作为核，在该核上被覆上述金属、金属粒子、碳而得的物质。在(e)导电性粒子是将塑料作为核，在该核上被覆上述金属、金属粒子、碳而得的物质、或热熔融金属粒子的情况下，由于通过加热加压而具有变形性，因此在连接时与电极的接触面积增加，可靠性提高，因而是优选的。
此外，这些(e)导电性粒子的表面进一步用高分子树脂等被覆而得的微粒，可以抑制当增加导电性粒子的含量时由粒子彼此接触所引起的短路、提高电极电路间的绝缘性，因此可以适当地将其单独使用或与(e)导电性粒子混合使用。
关于该(e)导电性粒子的平均粒径，从分散性、导电性的观点出发，优选为1～18μm。在含有这样的(e)导电性粒子的情况下，粘接剂组合物可以优选作为各向异性导电性粘接剂使用。
对粘接剂组合物中的(e)导电性粒子的含量没有特别地限制，相对于粘接剂组合物总体积优选为0.1～30体积％，更优选为0.1～10体积％。如果其值低于0.1体积％，则导电性倾向于降低，如果超过30体积％，则电路的短路倾向于容易发生。另外，体积％取决于23℃的固化前的各成分的体积，但各成分的体积可以利用比重由重量换算成体积。此外，也可以通过在量筒等中加入在不使该成分溶解或溶胀的情况下会使该成分良好润湿的适当溶剂(水、醇等)，在其中添加该成分，将增加了的体积作为该成分的体积而求出。
此外，关于本实施方式的粘接剂组合物，为了控制固化速度、赋予储存稳定性，可以添加稳定剂。作为这样的稳定剂，没有特别地限制，可以使用公知的化合物，优选为苯醌、氢醌等醌衍生物；4-甲氧基苯酚、4-叔丁基儿茶酚等酚衍生物；2，2，6，6-四甲基哌啶-1-氧基、4-羟基-2，2，6，6-四甲基哌啶-1-氧基等氨基氧基衍生物；四甲基哌啶基甲基丙烯酸酯等受阻胺衍生物等。
稳定剂的含量相对于粘接剂组合物100质量份优选为0.01～30质量份，更优选为0.05～10质量份。在含量低于0.01质量份的情况下，不易控制固化速度、不易赋予储存稳定性，在超过30质量份的情况下，容易对与其它成分的相容性带来不良影响。
此外，可以在本实施方式的粘接剂组合物中适当添加以烷氧基硅烷衍生物、硅氮烷衍生物为代表的偶联剂、密合性改进剂和流平剂等粘接助剂。作为偶联剂，具体而言，优选下述通式(P)所示的化合物。粘接助剂既可以单独使用也可以2种以上化合物混合使用。
[化20]
[式(P)中，R20，R21和R22各自独立地表示氢原子、碳原子数1～5的烷基、碳原子数1～5的烷氧基、碳原子数1～5的烷氧基羰基或芳基，R23表示(甲基)丙烯酰基、乙烯基、异氰酸酯基、咪唑基、巯基、氨基、甲基氨基、二甲基氨基、苄基氨基、苯基氨基、环己基氨基、吗啉基、哌嗪基、脲基或缩水甘油基，q表示1～10的整数。]
本实施方式的粘接剂组合物，为了缓和应力和提高粘接性，可以合并使用橡胶成分。橡胶成分是指在原本的状态下显示橡胶弹性(JISK6200)的成分或通过反应而显示橡胶弹性的成分。橡胶成分在室温(25℃)既可以是固体也可以是液体，从提高流动性的观点出发优选液体。作为橡胶成分，优选具有聚丁二烯骨架的化合物。橡胶成分可以具有氰基、羧基、羟基、(甲基)丙烯酰基或吗啉基。此外，从提高粘接性的观点出发，优选侧链或末端包含作为高极性基的氰基、羧基的橡胶成分。另外，即使是具有聚丁二烯骨架的化合物，在显示热塑性的情况下被分类到(a)热塑性树脂，在显示自由基聚合性的情况下被分类到(b)自由基聚合性化合物。
作为橡胶成分，具体而言，可列举聚异戊二烯、聚丁二烯、端羧基聚丁二烯、端羟基聚丁二烯、1，2-聚丁二烯、端羧基1，2-聚丁二烯、端羟基1，2-聚丁二烯、丙烯酸橡胶、丁苯橡胶、端羟基丁苯橡胶、丁腈橡胶、聚合物末端含有羧基、羟基、(甲基)丙烯酰基或吗啉基的丁腈橡胶、羧基化腈橡胶、端羟基聚(氧丙烯)、端烷氧基甲硅烷基聚(氧丙烯)、聚(氧亚丁基)二醇、聚烯烃二醇等。
此外，作为上述具有高极性基、在室温下为液体的橡胶成分，具体而言，可列举液体丁腈橡胶、在聚合物末端含有羧基、羟基、(甲基)丙烯酰基或吗啉基的液体丁腈橡胶、液体羧基化腈橡胶等，作为极性基的丙烯腈含量优选为10～60质量％。
这些橡胶成分既可以单独使用也可以2种以上化合物混合使用。
此外，为了缓和应力和提高粘接性，也可以在本实施方式的粘接剂组合物中添加有机微粒。有机微粒的平均粒径优选为0.05～1.0μm。另外，在有机微粒包含上述橡胶成分的情况下，不是分类到有机微粒而是分类到橡胶成分，在有机微粒包含上述(a)热塑性树脂的情况下，不是分类到有机微粒而是分类到(a)热塑性树脂。
作为有机微粒，具体而言，可列举由聚异戊二烯、聚丁二烯、端羧基聚丁二烯、端羟基聚丁二烯、1，2-聚丁二烯、端羧基1，2-聚丁二烯、丙烯酸橡胶、丁苯橡胶、丁腈橡胶、聚合物末端含有羧基、羟基、(甲基)丙烯酰基或吗啉基的丁腈橡胶、羧基化腈橡胶、端羟基聚(氧丙烯)、端烷氧基甲硅烷基聚(氧丙烯)、聚(氧亚丁基)二醇、聚烯烃二醇(甲基)丙烯酸烷基酯-丁二烯-苯乙烯共聚物、(甲基)丙烯酸烷基酯-有机硅共聚物或有机硅(甲基)-丙烯酸共聚物或复合体形成的有机微粒。
这些有机微粒既可以单独使用也可以2种以上化合物合并使用。
本实施方式的粘接剂组合物的断裂伸长率优选为300～500％，更优选为300～450％。通过使断裂伸长率在上述范围内，可以赋予充分的挠性，即使是具有有机基材的粘附体(聚酰亚胺、PET、PC、PEN等)，也可以追随它们的变形，并可以提高电路部件之间的粘接强度，获得优异的连接可靠性。如果断裂伸长率小于300％，则不能赋予充分的挠性，倾向于不易追随粘附体的变形，如果大于500％，则挠性过大，电路部件之间的粘接强度倾向于容易降低。
认为断裂伸长率可以通过使用由脂肪族系或芳香族系的二异氰酸酯和脂肪族系的二醇所得的聚氨酯(甲基)丙烯酸酯来调整。例如，如果使上述聚氨酯(甲基)丙烯酸酯的含量变多，则断裂伸长率倾向于变大。此外，如果上述聚氨酯(甲基)丙烯酸酯的重均分子量变大，则断裂伸长率也倾向于变大。此外，如果热塑性树脂的重均分子量高且Tg低，则断裂伸长率倾向于变大。此外，自由基聚合性化合物中的上述聚氨酯(甲基)丙烯酸酯所占的比例高时，断裂伸长率倾向于变大。此外，加入橡胶成分时，断裂伸长率倾向于变大。此外，如果有机微粒、无机填料的含量低，则断裂伸长率倾向于变大。
本实施方式的粘接剂组合物在200℃的储能模量优选为0.5～5MPa，更优选为0.5～3.5MPa。认为通过使在200℃的储能模量在上述范围内，可以兼有充分的挠性和交联密度，粘接剂组合物的粘附体和粘接剂组合物界面的应力得到缓和。因此，可以使电路部件之间的粘接强度提高，并且即使在长时间的可靠性试验之后也可以保持稳定的性能。如果储能模量小于0.5MPa或大于5MPa，则倾向于不易兼有充分的连接强度和良好的连接可靠性。
本实施方式的粘接剂组合物，在常温下为液体的情况下，可以以糊状使用。在室温下为固体的情况下，既可以加热后使用，也可以使用溶剂糊化。作为可以使用的溶剂，优选与粘接剂组合物和添加剂没有反应性且显示充分的溶解性的溶剂，优选在常压下的沸点为50～150℃的溶剂。在沸点低于50℃的情况下，如果在室温下放置，则很可能挥发，倾向于难以在开放体系中使用。此外，如果沸点超过150℃，则难以使溶剂挥发，经常对粘接后的可靠性带来不良影响。
此外，本实施方式的粘接剂组合物也可以形成膜状使用。可以将在粘接剂组合物中根据需要通过加入溶剂等方式得到的溶液涂布在氟树脂膜、聚对苯二甲酸乙二醇酯膜、脱模纸等剥离性基材上，或使上述溶液浸渍无纺布等基材而载置在剥离性基材上，除去溶剂等而作为膜使用。如果将粘接剂组合物以膜的形状使用，则从操作性等观点出发是更便利的。
本实施方式的粘接剂组合物可以合并使用加热和加压使其粘接。加热温度优选为100～200℃的温度。压力优选在不对粘附体造成损伤的范围内，一般优选为0.1～10MPa。这些加热和加压优选在0.5秒～120秒的范围内进行，也可以在120～190℃、3MPa、10秒的加热下使其粘接。
本实施方式的粘接剂组合物可以作为热膨胀系数不同的异种粘附体的粘接剂使用。具体而言，可以作为以各向异性导电粘接剂、银糊料、银膜等为代表的电路连接材料、CSP用弹性体、CSP用底部填充材料、LOC胶带等为代表的半导体元件粘接材料使用。
(第2实施方式)
此外，本发明的第2实施方式涉及的粘接剂组合物的特征在于，其是用于连接主面上具有第一连接端子的第一电路部件和主面上具有第二连接端子的第二电路部件的粘接剂组合物，包含(a)热塑性树脂、(b)自由基聚合性化合物和(c)自由基聚合引发剂，(b)自由基聚合性化合物含有聚氨酯(甲基)丙烯酸酯，断裂伸长率为300～500％。
通过使上述第2实施方式涉及的粘接剂组合物含有上述各成分，(b)自由基聚合性化合物含有聚氨酯(甲基)丙烯酸酯，断裂伸长率为300～500％，可以赋予粘接剂组合物以充分的挠性，追随粘附体(聚酰亚胺、PET、PC、PEN等)的变形，因此可以提高电路部件之间的粘接强度，获得优异的连接可靠性。上述粘接剂组合物的断裂伸长率更优选为300～450％。
在上述第2实施方式涉及的粘接剂组合物中，关于(a)热塑性树脂和(c)自由基聚合引发剂，使用与上述第1实施方式涉及的粘接剂组合物同样的物质。此外，(b)自由基聚合性化合物，虽然在所含有的聚氨酯(甲基)丙烯酸酯的临界表面张力没有特别限制这点上是不同的，但与第1实施方式涉及的粘接剂组合物同样地，所含有的聚氨酯(甲基)丙烯酸酯的临界表面张力优选为20～40mN/m，更优选为20～35mN/m，进一步优选为20～33mN/m。此外，关于在200℃的储能模量，也与上述第1实施方式涉及的粘接剂组合物同样地，优选为0.5～5MPa，更优选为0.5～3.5MPa。
上述第2实施方式涉及的粘接剂组合物，与第1实施方式涉及的粘接剂组合物同样地，优选包含(d)具有磷酸基的乙烯基化合物。通过包含(d)具有磷酸基的乙烯基化合物，可以使粘接剂组合物对金属基材的粘接性提高。此外，可以获得对具有由金属、ITO、IZO等所构成的连接端子的电路部件的优异粘接强度。
此外，在上述第2实施方式涉及的粘接剂组合物中，与第1实施方式涉及的粘接剂组合物同样地，可以添加(e)导电性粒子、稳定剂、偶联剂、粘接助剂、橡胶成分和有机微粒。
上述第2实施方式涉及的粘接剂组合物，关于(a)热塑性树脂、(b)自由基聚合性化合物和(c)自由基聚合引发剂，优选具有与第1实施方式涉及的粘接剂组合物同样的范围的含量。此外，在含有(d)具有磷酸基的乙烯基化合物、(e)导电性粒子、稳定剂、偶联剂、粘接助剂、橡胶成分和有机微粒的情况下，关于这些成分也优选具有与第1实施方式涉及的粘接剂组合物同样的范围的含量。
本发明的第1实施方式或第2实施方式涉及的粘接剂组合物作为用于连接主面上具有第一连接端子的第一电路部件和主面上具有第二连接端子的第二电路部件的粘接剂组合物使用。这里，上述第一电路部件和/或上述第二电路部件优选由包含玻璃化转变温度为200℃以下的热塑性树脂的基材构成，上述第一连接端子和/或上述第二连接端子优选由ITO和/或IZO所构成。作为玻璃化转变温度为200℃以下的热塑性树脂，没有特别限制，可列举例如，聚对苯二甲酸乙二醇酯、聚碳酸酯和聚萘二甲酸乙二醇酯等。
接下来，对使用了上述的本实施方式的粘接剂组合物的电路部件的连接结构体进行说明。图1是显示使用了不含有(e)导电性粒子的本实施方式的粘接剂组合物的、电路部件的连接结构体的一个实施方式的剖面示意图。图2是显示在制作图1所示的电路部件的连接结构体之前的第一电路部件、第二电路部件和粘接剂组合物(不含有导电性粒子)的剖面示意图。
图1所示的电路部件的连接结构体100包括：在第一电路基板31的主面31a上具有第一连接端子32的第一电路部件30、在第二电路基板41的主面41a上具有第二连接端子42的第二电路部件40、以第一连接端子32与第二连接端子42相对的方式连接第一电路基板31的主面31a和第二电路基板41的主面41a的连接部件10C。第一连接端子32和第二连接端子42彼此通过接触而被电连接。此外，连接部件10C包含本实施方式的粘接剂组合物10的固化物。
图1所示的电路部件的连接结构体100例如可以如下制造。
首先，如图2所示，准备第一电路部件30、第二电路部件40和成型为膜状的粘接剂组合物10。接下来，将粘接剂组合物10放置在第二电路部件40中的形成有第二连接端子42的主面41a上，然后，在粘接剂组合物10上以第一连接端子32与第二连接端子42相对的方式放置第一电路部件30。接着，一边隔着第一电路部件30和第二电路部件40加热粘接剂组合物10一边使其固化，同时在与主面31a、41a垂直的方向加压，在第一和第二电路部件30、40之间形成连接部件10C，从而获得图1的电路部件的连接结构体100。
图3是显示使用了含有(e)导电性粒子的本实施方式的粘接剂组合物的电路部件的连接结构体的一个实施方式的剖面示意图。图4是显示在制作图3所示的电路部件的连接结构体之前的第一电路部件、第二电路部件和粘接剂组合物(含有导电性粒子)的剖面示意图。
图3所示的电路部件的连接结构体200包括：第一电路基板31的主面31a上具有第一连接端子32的第一电路部件30、第二电路基板41的主面41a上具有第二连接端子42的第二电路部件40、以第一连接端子32与第二连接端子42相对的方式连接第一电路基板31的主面31a和第二电路基板41的主面41a的连接部件20C。另外，连接部件20C是在粘接剂组合物的除了导电性粒子以外的成分21中分散有导电性粒子22的粘接剂组合物20的固化物(即，在粘接剂组合物的除了导电性粒子以外的成分的固化物21C中分散有导电性粒子22的物质)，在相对的第一连接端子32和第二连接端子42之间，通过将导电性粒子22与两连接端子接触，从而介由导电性粒子22将两连接端子电连接。
图3所示的电路部件的连接结构体200，例如如图4所示，可以通过准备第一电路部件30、第二电路部件40和成型为膜状的粘接剂组合物20，利用与获得上述的电路部件的连接结构体100同样的方法来制造。
这里，第一电路部件30和第二电路部件40中的至少一个优选由含有聚对苯二甲酸乙二醇酯、聚碳酸酯和聚萘二甲酸乙二醇酯等玻璃化转变温度为200℃以下的热塑性树脂的基材构成。即，优选第一电路基板31和第二电路基板41中的至少一个含有聚对苯二甲酸乙二醇酯、聚碳酸酯和聚萘二甲酸乙二醇酯等玻璃化转变温度为200℃以下的热塑性树脂。如果第一电路部件30和第二电路部件40中的至少一个是由含有选自聚对苯二甲酸乙二醇酯、聚碳酸酯和聚萘二甲酸乙二醇酯中的至少1种材料的基材构成的电路部件，则可提高与粘接剂组合物的润湿性，进一步提高粘接强度。因此，这样的电路部件的连接结构体可以获得更优异的连接可靠性。
另外，第一电路部件30和第二电路部件40中的一个或两个可以由不含有聚对苯二甲酸乙二醇酯、聚碳酸酯和聚萘二甲酸乙二醇酯等玻璃化转变温度为200℃以下的热塑性树脂的基材构成。作为形成这样的电路部件的基材，可以使用包含半导体、玻璃、陶瓷等无机物的基材、包含聚酰亚胺等有机物的基材、使玻璃/环氧树脂等无机物与有机物组合所得的基材等。
此外，第一连接端子32和第二连接端子42中的至少一个优选由选自ITO和IZO中的至少1种所构成。ITO和IZO由于容易蚀刻且图案加工性优异，因此优选作为连接端子。而且，通过使用本实施方式的粘接剂组合物，可以充分地抑制由ITO和/或IZO构成的连接端子的腐蚀。
另外，第一连接端子32和第二连接端子42中的一个或两个可以由除了ITO和IZO以外的材料所构成。作为这样的连接端子，可以使用包含铜、银、铝、金、钯、镍和它们的合金等金属的连接端子。
另外，作为连接部件使用的本实施方式的粘接剂组合物，不需要完全固化(在规定固化条件下可以达到的最高度的固化)，只要产生上述特性即可，可以是部分固化的状态。
实施例
以下，基于实施例具体地说明本发明，但本发明不限定于此。
<热塑性树脂>
(聚酯型聚氨酯的准备)
聚酯型聚氨酯树脂(东洋纺株式会社制，UR-8200(商品名))使用了树脂组分30质量％的甲基乙基酮与甲苯的1∶1混合溶剂溶解品。
(苯氧树脂的准备)
苯氧树脂(东都化成株式会社制，YP-50(商品名))是将树脂40质量份溶解在甲基乙基酮60质量份中而制成固体成分40质量％的溶液。
(乙烯-乙酸乙烯酯共聚物的准备)
乙烯-乙酸乙烯酯共聚物(三井杜邦聚合化学制，EV40W(商品名))使用了树脂组分30质量％的甲苯溶解品。
<自由基聚合性化合物>
(聚氨酯丙烯酸酯(UA1)的合成)
在具备搅拌机、温度计、具备氯化钙干燥管的回流冷却管、氮气导入管的反应容器中添加丙烯酸2-羟乙酯(Aldrich株式会社制)238质量份(2.05摩尔)、氢醌单甲基醚(Aldrich株式会社制)0.53质量份、数均分子量1000的聚(1，6-己二醇碳酸酯)(商品名：DURANOLT5652，旭化成化学株式会社制)2000质量份(2.00摩尔)、二丁基锡二月桂酸酯(Aldrich株式会社制)5.53质量份。充分地导入氮气，然后加热到70～75℃，经3小时均匀地滴加氢化二苯基甲烷二异氰酸酯(商品名：VESTANATH12MD，Degussa公司制)787质量份(3.00摩尔)，使其反应。滴加结束后，使其反应11小时，通过IR测定确认异氰酸酯消失，结束反应，从而获得了聚氨酯丙烯酸酯。所得的聚氨酯丙烯酸酯(UA1)的临界表面张力为24mN/m，重均分子量为13500，粘度为2500Pa·s。
(聚氨酯丙烯酸酯(UA2)的合成)
在具备搅拌机、温度计、具备氯化钙干燥管的回流冷却管、氮气导入管的反应容器中添加入丙烯酸2-羟乙酯(Aldrich株式会社制)238质量份(2.05摩尔)、氢醌单甲基醚(Aldrich株式会社制)0.53质量份、数均分子量1000的聚(1，6-己二醇碳酸酯)(商品名：DURANOLT5652，旭化成化学株式会社制)1000质量份(2.00摩尔)、二丁基锡二月桂酸酯(Aldrich株式会社制)5.53质量份。充分地导入氮气，然后加热到70～75℃，经3小时均匀地滴加氢化二苯基甲烷二异氰酸酯(商品名：VESTANATH12MD，Degussa公司制)787质量份(3.00摩尔)，使其反应。滴加结束后，使其反应13小时，通过IR测定确认异氰酸酯消失，结束反应，从而获得了聚氨酯丙烯酸酯。所得的聚氨酯丙烯酸酯(UA2)的临界表面张力为23mN/m，重均分子量为15500，粘度为4100Pa·s。
(聚氨酯丙烯酸酯(UA3)的合成)
在具备搅拌机、温度计、具备氯化钙干燥管的回流冷却管、氮气导入管的反应容器中添加入丙烯酸2-羟乙酯(Aldrich株式会社制)238质量份(2.05摩尔)、氢醌单甲基醚(Aldrich株式会社制)0.53质量份、数均分子量2000的聚己内酯二醇(商品名：Placcel220，大赛璐化学工业株式会社制)4000质量份(2.00摩尔)、二丁基锡二月桂酸酯(Aldrich株式会社制)5.53质量份。充分地导入氮气，然后加热到70～75℃，经3小时均匀地滴加异佛尔酮二异氰酸酯(Aldrich株式会社制)666质量份(3.00摩尔)，使其反应。滴加结束后，使其反应12小时，通过IR测定确认异氰酸酯消失，结束反应，从而获得了聚氨酯丙烯酸酯。所得的聚氨酯丙烯酸酯(UA3)的临界表面张力为27mN/m，重均分子量为13800，粘度为650Pa·s。
(聚氨酯丙烯酸酯(UA4)的合成)
在具备搅拌机、温度计、具备氯化钙干燥管的回流冷却管、氮气导入管的反应容器中，将3-甲基-1，5-戊二醇1650质量份(14摩尔)和癸二酸2023质量份(10摩尔)加入反应器中，在常压下充分地导入氮气，然后一边在约170℃将所生成的水从体系内蒸馏除去，一边进行酯化反应。在聚酯的酸值变为0.3mgKOH/g以下的时刻，通过真空泵逐渐地升高真空度，使反应结束。这样获得的聚酯二醇具有数均分子量1000。
然后，在具备搅拌机、温度计、具备氯化钙干燥管的回流冷却管、氮气导入管的反应容器中添加丙烯酸2-羟乙酯(Aldrich株式会社制)238质量份(2.05摩尔)、氢醌单甲基醚(Aldrich株式会社制)0.53质量份、上述获得的聚酯二醇2000质量份(2.00摩尔)、二丁基锡二月桂酸酯(Aldrich株式会社制)5.53质量份。充分地导入氮气，然后加热到70～75℃，经3小时均匀地滴加异佛尔酮二异氰酸酯(Aldrich株式会社制)666质量份(3.00摩尔)，使其反应。滴加结束后，使其反应约15小时，通过IR测定确认异氰酸酯消失，结束反应，从而获得了聚氨酯丙烯酸酯。所得的聚氨酯丙烯酸酯(UA4)的临界表面张力为43mN/m，重均分子量为18500，粘度为4800Pa·s。
(聚氨酯丙烯酸酯(UA5)的合成)
在具备搅拌机、温度计、具备氯化钙干燥管的回流冷却管、氮气导入管的反应容器中添加丙烯酸2-羟乙酯(Aldrich株式会社制)238质量份(2.05摩尔)、氢醌单甲基醚(Aldrich株式会社制)0.53质量份、数均分子量1000的聚四亚甲基醚乙二醇(商品名：保土谷化学工业株式会社制，TG1000)2000质量份(2.00摩尔)、二丁基锡二月桂酸酯(Aldrich株式会社制)5.53质量份。充分地导入氮气，然后加热到70～75℃，经3小时均匀地滴加异佛尔酮二异氰酸酯(Aldrich株式会社制)666质量份(3.00摩尔)，使其反应。滴加结束后，使其反应进行13小时。通过IR测定确认异氰酸酯消失，结束反应，从而获得了聚氨酯丙烯酸酯。所得的聚氨酯丙烯酸酯(UA5)的临界表面张力为17mN/m，重均分子量为14500，粘度为2900Pa·s。
(聚氨酯丙烯酸酯(UA6)的合成)
在具备搅拌机、温度计、具备氯化钙干燥管的回流冷却管、氮气导入管的反应容器中，将3-甲基-1，5-戊二醇1650质量份(14摩尔)和癸二酸2023质量份(10摩尔)加入反应器中，在常压下充分地导入氮气，然后一边在约170℃将所生成的水从体系内蒸馏除去，一边进行酯化反应。在聚酯的酸值变为0.3mgKOH/g以下的时刻，通过真空泵逐渐地升高真空度，使反应结束。这样获得的聚酯二醇具有数均分子量1000。
然后，在具备搅拌机、温度计、具备氯化钙干燥管的回流冷却管、氮气导入管的反应容器中添加丙烯酸2-羟乙酯(Aldrich株式会社制)238质量份(2.05摩尔)、氢醌单甲基醚(Aldrich株式会社制)0.53质量份、上述获得的聚酯二醇2500质量份(2.50摩尔)、二丁基锡二月桂酸酯(Aldrich株式会社制)5.53质量份。充分地导入氮气，然后加热到70～75℃，经3小时均匀地滴加异佛尔酮二异氰酸酯(Aldrich株式会社制)666质量份(3.00摩尔)，使其反应。滴加结束后，使其反应约17小时，通过IR测定确认异氰酸酯消失，结束反应，从而获得了聚氨酯丙烯酸酯。所得的聚氨酯丙烯酸酯(UA6)的临界表面张力为41mN/m，重均分子量为23500，粘度为6800Pa·s。
(聚氨酯丙烯酸酯(UA7)的合成)
在具备搅拌机、温度计、具备氯化钙干燥管的回流冷却管、氮气导入管的反应容器中添加丙烯酸2-羟乙酯(Aldrich株式会社制)238质量份(2.05摩尔)、氢醌单甲基醚(Aldrich株式会社制)0.53质量份、数均分子量1000的聚四亚甲基醚二醇(商品名：保土谷化学工业株式会社制，TG1000)2500质量份(2.50摩尔)、二丁基锡二月桂酸酯(Aldrich株式会社制)5.53质量份。充分地导入氮气，然后加热到70～75℃，经3小时均匀地滴加异佛尔酮二异氰酸酯(Aldrich株式会社制)666质量份(3.00摩尔)，使其反应。滴加结束后，使其反应15小时。通过IR测定确认异氰酸酯消失，结束反应，从而获得了聚氨酯丙烯酸酯。所得的聚氨酯丙烯酸酯(UA7)的临界表面张力为16mN/m，重均分子量为20400，粘度为3500Pa·s。
(异氰脲酸改性2官能丙烯酸酯(M-215)的准备)
准备异氰脲酸改性2官能丙烯酸酯(东亚合成株式会社制，M-215(商品名))。
(具有磷酸基的乙烯基化合物(P-2M)的准备)
准备2-(甲基)丙烯酰氧基乙基磷酸酯(商品名：lightesterP-2M，共荣社化学株式会社制)。
<自由基聚合引发剂>
准备作为自由基聚合引发剂的过氧化二苯甲酰(商品名：NiparBW，日油株式会社制)。
<导电性粒子>
(导电性粒子的制作)
在将聚苯乙烯作为核的粒子的表面设置厚度0.2μm的镍层，在该镍层的外侧设置厚度0.02μm的金层，从而制作平均粒径10μm、比重2.5的导电性粒子。
[实施例1～7、参考例8～12和比较例1～5]
按照表2所示的固体质量比配合热塑性树脂、自由基聚合性化合物和自由基聚合引发剂，然后使导电性粒子1.5体积％配合分散，从而获得了粘接剂组合物。使用涂覆装置将所得的粘接剂组合物涂布在厚度80μm的氟树脂膜上，通过70℃、10分钟的热风干燥来获得粘接剂层的厚度为20μm的膜状粘接剂组合物。
[表2]
〔断裂伸长率、储能模量、连接电阻、粘接强度的测定〕
使实施例1～7、参考例8～12和比较例1～5的膜状粘接剂组合物介于在聚酰亚胺膜上具有500根线宽25μm、间距50μm、厚度8μm的铜电路的挠性电路板(FPC)和形成有0.2μm的ITO薄层的玻璃(厚度1.1mm、表面电阻20Ω/□)之间。使用热压接装置(加热方式：恒热型，东丽工程社制)将其在160℃、3MPa的条件下加热加压10秒，连接涉及宽2mm，从而制作连接体。在刚粘接后和在85℃、85％RH的高温高湿槽中保持240小时后(试验后)用万用表测定该连接体的相邻电路间的电阻值。电阻值以37处相邻电路间的电阻的平均值表示。
此外，按照JIS-Z0237通过90度剥离法测定各连接体的粘接强度，进行评价。这里，粘接强度的测定装置使用东洋鲍德温株式会社制tensilonUTM-4(剥离速度50mm/分钟，25℃)。
此外，膜状粘接剂组合物的断裂伸长率如下测定：将膜状的粘接剂组合物在180℃加热固化1小时，用英斯特朗公司制材料试验机“microtester5548”(拉伸速度50mm/分钟，25℃)对所得的样品进行测定。此外，膜状粘接剂组合物的储能模量如下测定：将膜状的粘接剂组合物在180℃加热固化1小时，用TA仪器公司制粘弹性分析器“RSA-3”(升温速度5℃/分钟，频率10Hz，测定温度-150～300℃)对所得的样品进行测定。如上进行的膜状粘接剂组合物的断裂伸长率、储能模量、连接电阻和粘接强度的测定的结果示于下表3。
[表3]
由实施例1～7获得的粘接剂组合物含有(a)、(b)、(c)和(d)成分，通过使用包含具有特定范围的临界表面张力的聚氨酯(甲基)丙烯酸酯作为(b)成分的粘接剂组合物，与使用了包含特定范围外的临界表面张力的粘接剂组合物的参考例8～12和比较例1～5相比，在加热温度160℃下，在刚粘接后和在85℃、85％RH的高温高湿槽中保持240小时后(试验后)均显示出约2.6Ω以下的良好的连接电阻和600N/m以上的良好的粘接强度。此外，膜状粘接剂组合物的断裂伸长率和储能模量也显示出良好的值。
另一方面，由比较例1～5获得的粘接剂组合物，在刚粘接后和在85℃、85％RH的高温高湿槽中保持240小时后(试验后)均显示出低粘接强度。此外，由比较例4和5获得的粘接剂组合物，在85℃、85％RH的高温高湿槽中保持240小时后(试验后)的连接电阻高，粘接强度也低。此外，膜状粘接剂组合物的断裂伸长率或储能模量也显示出良好的值，但在比较例2和3中断裂伸长率显示出小于良好的范围的值，在比较例4和5中断裂伸长率显示出大于良好的范围的值。此外，在比较例2和3中储能模量也显示出大于良好的范围的值。
此外，由参考例8～12获得的粘接剂组合物含有(a)、(b)和(c)成分，包含聚氨酯(甲基)丙烯酸酯作为(b)成分，使用具有特定范围的断裂伸长率的粘接剂组合物，由此，与断裂伸长率在范围外的比较例2～5相比，连接电阻与粘接强度之间的平衡好。因此认为通过使粘接剂组合物的断裂伸长率在特定范围内，即使不使用具有特定范围的临界表面张力的聚氨酯(甲基)丙烯酸酯，也可以向粘接剂组合物赋予挠性，并可以获得平衡好的特性。
此外，使实施例1、2、4、5和参考例10以及比较例5的膜状粘接剂组合物介于在聚酰亚胺膜上具有80根线宽150μm、间距300μm、厚度18μm的铜电路的FPC与在PET膜(厚度0.1mm、Tg120℃)、PC膜(厚度0.1mm、Tg150℃)和PEN膜(厚度0.1mm，Tg160℃)膜上形成有线宽150μm、间距300μm、厚度10μm的Ag糊料电路的基板之间。使用热压接装置(加热方式：恒热型，东丽工程社制)将它们分别在150℃、2MPa的条件下加热加压10秒，压接涉及宽2mm，从而制作连接体。
此外，将各连接体的粘接强度与上述方法同样地测定。如上进行的膜状粘接剂组合物的粘接强度的测定的结果示于下表4。
[表4]
由实施例13～16所得的粘接剂组合物，对任何基材，在加热温度150℃下，在刚粘接后和在85℃、85％RH的高温高湿槽中保持240小时后(试验后)都显示出560N/m以上的良好的粘接强度。与此相对，在比较例6中，在刚粘接后和在85℃、85％RH的高温高湿槽中保持240小时后(试验后)，粘接强度变低。另外，实施例17不如实施例13～16，但与比较例6相比改善了粘接强度。
产业可利用性
根据本发明，可以提供即使在低温的固化条件下也可以获得优异的粘接强度、即使在长时间的可靠性试验(高温高湿试验)之后也可以保持稳定的性能(粘接强度、连接电阻)的粘接剂组合物、使用了该粘接剂组合物的电路部件的连接结构体、连接结构体的制造方法、以及粘接剂组合物的应用。
符号说明
10、20为粘接剂组合物；
10C、20C为连接部件；
21为不包含导电性粒子的粘接剂组合物；
22为导电性粒子；
21C为不包含导电性粒子的粘接剂组合物的固化物；
30为第一电路部件；
31为第一电路基板；
31a为主面；
32为第一连接端子；
40为第二电路部件；
41为第二电路基板；
41a为主面；
42为第二连接端子；
100、200为电路部件的连接结构体。

Claims (31)

1.一种粘接剂组合物，其是用于连接主面上具有第一连接端子的第一电路部件和主面上具有第二连接端子的第二电路部件的粘接剂组合物，
所述粘接剂组合物含有(a)热塑性树脂、(b)自由基聚合性化合物、(c)自由基聚合引发剂和(d)具有磷酸基的乙烯基化合物，
所述(b)自由基聚合性化合物包含具有23～27mN/m的临界表面张力的聚氨酯(甲基)丙烯酸酯。
2.根据权利要求1所述的粘接剂组合物，其中，所述聚氨酯(甲基)丙烯酸酯在25℃时的粘度为600～5000Pa·s。
3.根据权利要求1或2所述的粘接剂组合物，其中，所述聚氨酯(甲基)丙烯酸酯的重均分子量为10000以上且小于25000。
4.根据权利要求1或2所述的粘接剂组合物，其中，所述聚氨酯(甲基)丙烯酸酯是通过脂肪族系二异氰酸酯和脂肪族二醇的缩合反应来获得的。
5.根据权利要求4所述的粘接剂组合物，其中，所述脂肪族系二异氰酸酯是丁二异氰酸酯、己二异氰酸酯、赖氨酸二异氰酸酯、2-甲基戊烷-1，5-二异氰酸酯、3-甲基戊烷-1，5-二异氰酸酯、2，2，4-三甲基六亚甲基-1，6-二异氰酸酯、2，4，4-三甲基六亚甲基-1，6-二异氰酸酯、异佛尔酮二异氰酸酯、环己基二异氰酸酯、氢化苯二亚甲基二异氰酸酯、氢化二苯基甲烷二异氰酸酯或者氢化三甲基苯二亚甲基二异氰酸酯。
6.根据权利要求4所述的粘接剂组合物，其中，所述脂肪族二醇为：将乙二醇、丙二醇、1，2-丙二醇、1，3-丙二醇、1，3-丁二醇、1，4-丁二醇、新戊二醇、1，2-戊二醇、1，4-戊二醇、1，5-戊二醇、2，4-戊二醇、2-甲基-2，4-戊二醇、2，4-二甲基-2，4-戊二醇、2，2，4-三甲基-1，3-戊二醇、1，2-己二醇、1，5-己二醇、1，6-己二醇、2，5-己二醇、2-乙基-1，3-己二醇、2，5-二甲基-2，5-己二醇、1，2-辛二醇、1，8-辛二醇、1，7-庚二醇、1，9-壬二醇、1，2-癸二醇、1，10-癸二醇、1，12-癸二醇、十二烷二醇、频哪醇、1，4-丁炔二醇、三乙二醇、二甘醇、双丙甘醇或环己烷二甲醇即饱和的低分子二醇类，由至少1种以上的所述低分子二醇类与碳酰氯反应所得的聚碳酸酯二醇类，以至少1种以上的所述低分子二醇类作为引发剂将选自环氧乙烷、环氧丙烷、表氯醇中的至少1种加成聚合所得的聚醚二醇类，与己二酸、3-甲基己二酸、2，2，5，5-四甲基己二酸、马来酸、富马酸、琥珀酸、2，2-二甲基琥珀酸、2-乙基-2-甲基琥珀酸、2，3-二甲基琥珀酸、草酸、丙二酸、甲基丙二酸、乙基丙二酸、丁基丙二酸、二甲基丙二酸、戊二酸、2-甲基戊二酸、3-甲基戊二酸、2，2-二甲基戊二酸、3，3-二甲基戊二酸、2，4-二甲基戊二酸、庚二酸、辛二酸、壬二酸或癸二酸的二元酸或所述二元酸的酸酐脱水缩合所得的聚酯二醇类；或者将环状酯化合物开环聚合所得的聚酯二醇类。
7.根据权利要求1或2所述的粘接剂组合物，其中，所述聚氨酯(甲基)丙烯酸酯的重均分子量为12000以上且低于20000。
8.根据权利要求1或2所述的粘接剂组合物，其中，所述聚氨酯(甲基)丙烯酸酯在25℃时的粘度为600～4500Pa·s。
9.根据权利要求1或2所述的粘接剂组合物，其中，所述聚氨酯(甲基)丙烯酸酯的配合量以所述粘接剂组合物总量为基准，为5～95质量％。
10.根据权利要求1或2所述的粘接剂组合物，其中，所述(d)具有磷酸基的乙烯基化合物是分子内具有至少一个以上(甲基)丙烯酰基的磷酸(甲基)丙烯酸酯化合物。
11.根据权利要求1或2所述的粘接剂组合物，其中，所述分子内具有至少一个以上(甲基)丙烯酰基的磷酸(甲基)丙烯酸酯化合物是下述通式(M)～(O)所示的化合物，
式(M)中，R15表示(甲基)丙烯酰氧基，R16表示氢原子或甲基，k和l各自独立地表示1～8的整数；另外，式中，R15彼此之间、R16彼此之间、k彼此之间和l彼此之间相同或不同，
式(N)中，R17表示(甲基)丙烯酰氧基，m和n各自独立地表示1～8的整数；另外，式中，R17彼此之间、m彼此之间和n彼此之间相同或不同，
式(O)中，R18表示(甲基)丙烯酰氧基，R19表示氢原子或甲基，o和p各自独立地表示1～8的整数；另外，式中，R19彼此之间和o彼此之间相同或不同。
12.根据权利要求1或2所述的粘接剂组合物，其中，所述(d)含有磷酸基的乙烯基化合物的含量，相对于所述(a)热塑性树脂100质量份为0.2～300质量份。
13.根据权利要求1或2所述的粘接剂组合物，其中，所述(b)自由基聚合性化合物的含量，相对于所述(a)热塑性树脂100质量份为50～250质量份。
14.根据权利要求1或2所述的粘接剂组合物，其中，在200℃时的储能模量为0.5～5MPa。
15.根据权利要求1或2所述的粘接剂组合物，其中，在200℃时的储能模量为0.5～3.5MPa。
16.根据权利要求1或2所述的粘接剂组合物，其中，所述(a)热塑性树脂含有选自由苯氧树脂、聚氨酯树脂、聚酯型聚氨酯树脂、聚乙烯醇缩丁醛树脂、丙烯酸树脂和聚酰亚胺树脂组成的组中的至少1种树脂。
17.根据权利要求1或2所述的粘接剂组合物，其中，所述(a)热塑性树脂的重均分子量为5,000～150,000。
18.根据权利要求1或2所述的粘接剂组合物，其中，所述(a)热塑性树脂的含量以所述粘接剂组合物总量为基准，为5～80质量％。
19.根据权利要求1或2所述的粘接剂组合物，其中，所述(c)自由基聚合引发剂为有机过氧化物或者偶氮化合物。
20.根据权利要求1或2所述的粘接剂组合物，其中，所述(c)自由基聚合引发剂的含量，相对于所述(a)热塑性树脂100质量份为0.1～500质量份。
21.根据权利要求1或2所述的粘接剂组合物，其中，还含有(e)导电性粒子。
22.一种电路部件的连接结构体，包括：主面上具有第一连接端子的第一电路部件、主面上具有第二连接端子的第二电路部件、和连接部件，
以所述第一连接端子与所述第二连接端子相对的方式，所述第一电路部件和所述第二电路部件介由所述连接部件而配置，并且所述第一连接端子和所述第二连接端子被电连接，
所述连接部件是权利要求1～21中的任一项所述的粘接剂组合物的固化物，
所述第一电路部件和/或所述第二电路部件由包含玻璃化转变温度为200℃以下的热塑性树脂的基材构成。
23.根据权利要求22所述的电路部件的连接结构体，其中，所述玻璃化转变温度为200℃以下的热塑性树脂是选自由聚对苯二甲酸乙二醇酯、聚碳酸酯和聚萘二甲酸乙二醇酯组成的组中的至少1种树脂。
24.根据权利要求22或23所述的电路部件的连接结构体，其中，
所述第一电路部件或所述第二电路部件中的一个电路部件由含有选自由聚对苯二甲酸乙二醇酯、聚碳酸酯和聚萘二甲酸乙二醇酯组成的组中的至少1种材料的基材构成，
所述第一电路部件或第二电路部件中的另一电路部件是聚酰亚胺树脂。
25.一种电路部件的连接结构体的制造方法，包括下述工序：
将主面上具有第一连接端子的第一电路部件和主面上具有第二连接端子的第二电路部件介由权利要求1～21中的任一项所述的粘接剂组合物以所述第一连接端子与所述第二连接端子相对的方式配置的工序，
将所述粘接剂组合物加热，使其固化，连接所述第一电路部件与所述第二电路部件的工序。
26.权利要求1～21中的任一项所述的粘接剂组合物作为电路连接材料的应用，所述电路连接材料用于连接主面上具有第一连接端子的第一电路部件和主面上具有第二连接端子的第二电路部件。
27.根据权利要求26所述的应用，其中，所述玻璃化转变温度为200℃以下的热塑性树脂是选自聚对苯二甲酸乙二醇酯、聚碳酸酯和聚萘二甲酸乙二醇酯组成的组中的至少1种树脂。
28.根据权利要求26或27所述的应用，其中，所述第一电路部件或所述第二电路部件中的一个电路部件由含有选自聚对苯二甲酸乙二醇酯、聚碳酸酯和聚萘二甲酸乙二醇酯组成的组中的至少1种材料的基材构成，
所述第一电路部件或所述第二电路部件中的另一电路部件是聚酰亚胺树脂。
29.权利要求1～21中的任一项所述的粘接剂组合物在电路连接材料的制造中的应用，所述电路连接材料用于连接主面上具有第一连接端子的第一电路部件和主面上具有第二连接端子的第二电路部件。
30.根据权利要求29所述的应用，其中，所述玻璃化转变温度为200℃以下的热塑性树脂是选自聚对苯二甲酸乙二醇酯、聚碳酸酯和聚萘二甲酸乙二醇酯组成的组中的至少1种树脂。
31.根据权利要求29或30所述的应用，其中，所述第一电路部件或所述第二电路部件中的一个电路部件由含有选自聚对苯二甲酸乙二醇酯、聚碳酸酯和聚萘二甲酸乙二醇酯组成的组中的至少1种材料的基材构成，
所述第一电路部件或所述第二电路部件中的另一电路部件是聚酰亚胺树脂。
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