CN1214455C - 电路连接用粘接剂、使用其的电路连接方法及电路连接结构体 - Google Patents
电路连接用粘接剂、使用其的电路连接方法及电路连接结构体 Download PDFInfo
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- CN1214455C CN1214455C CNB018082556A CN01808255A CN1214455C CN 1214455 C CN1214455 C CN 1214455C CN B018082556 A CNB018082556 A CN B018082556A CN 01808255 A CN01808255 A CN 01808255A CN 1214455 C CN1214455 C CN 1214455C
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Classifications
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- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
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- H01L21/04—Manufacture or treatment of semiconductor devices or of parts thereof the devices having potential barriers, e.g. a PN junction, depletion layer or carrier concentration layer
- H01L21/50—Assembly of semiconductor devices using processes or apparatus not provided for in a single one of the subgroups H01L21/06 - H01L21/326, e.g. sealing of a cap to a base of a container
- H01L21/60—Attaching or detaching leads or other conductive members, to be used for carrying current to or from the device in operation
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- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
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- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
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Abstract
一种电路连接用粘接剂,是介于具有相向的电路电极的基板间,对具有相向的电路电极的基板加压,在加压方向的电极间作电连接的电路连接用粘接剂,上述粘接剂是在其中含有酸当量为5至500(KOH毫克/克)的化合物的电路连接用粘接剂,以及介于具有相向的电路电极的基板间,对具有相向的电路电极的基板加压,在加压方向的电极间作电连接的电路连接用粘接剂,其特征为上述粘接剂具有第一粘接剂层及第二粘接剂层,第一粘接剂层的加压连接后的玻璃化转变温度(Tg)高于第二粘接剂层的加压连接后的Tg。
Description
技术领域
本发明涉及一种电路连接用粘接剂、使用该粘接剂的电路连接方法以及电路连接结构体。
背景技术
以往,液晶显示器与载带封装(TCP)或挠性印制电路(FPC)的连接,TCP或FPC与印刷电路板之间的连接是使用在粘接剂中分散有导电性粒子的各向异性导电粘接剂。而且,最近将半导体硅芯片安装于基板时,也已不用焊线法,而是将半导体硅芯片面朝下地直接安装于基板,进行所谓的倒装片(flip chip)安装,此时也开始采用各向异性导电粘接剂(日本专利特开昭59-120436号、特开昭60-191228号、特开平1-251787号、特开平7-90237号公报)。
然而,以往的各向异性导电粘接剂对于各种基板的粘接力不足,从而无法获得充分的连接可靠性。尤其是,无法充分、可靠地满足为了降低连接时对基板的伤害或位置的偏移以及提高生产效率而要求的连接温度的低温化和连接时间的缩短等。
发明内容
本发明是提供一种实现了连接温度的低温化、连接时间的缩短化的电路连接用粘接剂,及使用该粘接剂的电路连接方法以及使用该方法的电路连接结构体。
本发明之1是介于具有相向的电路电极的基板间,对具有相向的电路电极的基板加压,而在加压方向的电极间作电连接的电路连接用粘接剂,其特征为上述粘接剂含有酸当量按KOH毫克/克计为5至500的化合物。
本发明之2是本发明之1所述的电路连接用粘接剂,其特征为酸当量按KOH毫克/克计为5至500的化合物是含有至少一个羧基的化合物。
本发明之3是本发明之1或2所述的电路连接用粘接剂,其特征为还含有自由基聚合性物质。
本发明之4是本发明之1至3中的任意一项所述的电路连接用粘接剂,其特征为还含有导电粒子。
本发明之5是一种使电路连接用粘接剂介于具有相向的电路电极的基板间,对具有相向的电路电极的基板加压,使加压方向的电极间电连接的连接结构体,其特征为上述电路连接用粘接剂为本发明之1至4的任意一项所述的粘接剂。
本发明之6是介于具有相向的电路电极的基板间,对具有相向的电路电极的基板加压,而在加压方向的电极间作电连接的电路连接用粘接剂,其特征为上述粘接剂具有第一粘接剂层及第二粘接剂层,而第一粘接剂层的加压连接后的玻璃化转变温度(Tg)高于第二粘接剂层的加压连接后的Tg。
本发明之7是根据本发明之6所述的电路连接用粘接剂,其特征为第一粘接剂层的连接后的Tg为50至200℃,而第二粘接剂层的连接后的Tg为40至100℃,且第一粘接剂层的Tg较第二粘接剂层的连接后的Tg高5℃以上。
本发明之8是根据本发明之6或本发明之7所述的电路连接用粘接剂,其特征为第一粘接剂层以及第二粘接剂层中的至少一层含有导电粒子。
本发明之9是根据本发明之6至本发明之8任意一项所述的电路连接用粘接剂,其特征为第一粘接剂层和第二粘接剂层中的至少一层含有自由基聚合性物质。
本发明之10是根据本发明之6至本发明之9任意一项所述的电路连接用粘接剂,其特征为第一粘接剂层与第二粘接剂层的厚度比为,第一粘接剂层的厚度/第二粘接剂层的厚度=0.3至3.0。
本发明之11是根据本发明之6至本发明之10任意一项所述的电路连接用粘接剂,其特征为第一粘接剂层以及第二粘接剂层的至少一层含有酸当量按KOH毫克/克计为5至500的化合物。
本发明之12是,将本发明之6至本发明之11任意一项所述的电路连接用粘接剂介于具有相向的电路电极的基板间,对具有相向的电路电极的基板加压,在加压方向的电极间作电连接的方法,其特征为上述电路连接用粘接剂具有第一粘接剂层及第二粘接剂层,第一粘接剂层的加压连接后的Tg高于第二粘接剂层的加压连接后的Tg,而且Tg较高的第一粘接剂层是位于具有相向电路电极的基板中弹性率较高的基板侧。
本发明之13是,将本发明之6至本发明之11任意一项所述的电路连接用粘接剂介于具有相向的电路电极的基板间,对具有相向的电路电极的基板加压,在加压方向的电极间作电连接的连接结构体,其特征为上述粘接剂具有第一粘接剂层及第二粘接剂层,第一粘接剂层的加压连接后的Tg高于第二粘接剂层的加压连接后的Tg,而且Tg较高的第一粘接剂层是位于具有相向电路电极的基板中弹性率较高的基板侧面。
具体实施方式
本发明的电路连接用粘接剂以及使用该粘接剂的电路连接方法及电路连接结构体中,进行耐湿试验、冷热循环试验等各种可靠性试验后,也没有发生从基板上的脱落、剥离现象,所以不会使粘接力下降或连接电阻上升,呈现出优异的连接可靠性。
在本发明之1中,可使用用氢氧化钾滴定法测定的酸当量在5至500(KOH毫克/克)范围的化合物,理想的是使用含有羧基的化合物。酸当量如果小于5则看不出粘接力的上升,而如果大到超过500,则因粘接剂的吸水率变大,故耐湿可靠性降低。含有羧基的化合物是只要在分子内含有羧基的化合物就可以,没有特别的限制。而且对重均分子量也没有特别的限制,但理想的是化合物的重均分子量小于1,000,000。分子量若大于1,000,000则粘接剂的流动性下降。含有羧基的化合物的具体举例为,草酸、丙二酸等羧酸、以及在聚丁二烯、聚乙烯醇缩丁醛、(甲基)丙烯酸树脂、聚酰亚胺、聚酰胺、聚苯乙烯、聚乙烯醇缩甲醛树脂、聚酯树脂、二甲苯树脂、苯氧基树脂、聚氨酯树脂、尿素树脂等聚合物中导入羧基的化合物。在高分子中导入羧基时,可将含有羧基的化合物用作共聚成分,也可在聚合物合成之后再导入羧基。本发明中所使用的、在高分子中导入羧基后的化合物的配比量较好是1至80重量%,更好是5至70重量%。小于1重量%时粘接性差,而超过80重量%则流动性下降。
本发明中除了使用上述的含有羧基的化合物以外还使用苯乙烯—丁二烯—苯乙烯共聚物、苯乙烯-异戊二烯-苯乙烯共聚物等热可塑性树脂、或环氧树脂、(甲基)丙烯酸树脂、马来酰亚胺树脂、柠康酰亚胺树脂、降冰片烯酰亚胺树脂、酚类树脂等热固化性树脂,从耐热性或可靠性的观点出发理想的是使用热硬化性树脂,从低温固化性的观点是出发,使用(甲基)丙烯酸是树脂、马来酰亚胺树脂、柠康酰亚胺树脂、降冰片烯酰亚胺树脂的自由基聚合系是尤其理想的。
本发明之2的电路连接用粘接剂,是由第一粘接剂层以及第二粘接剂层所构成,其中第一粘接剂层的连接后的Tg必须高于第二粘接剂层的连接后的Tg。第一粘接剂层的Tg理想的是50至200℃,更理想为60至150℃。并且,第二粘接剂层的Tg在40至100℃,第一粘接剂层的Tg较第二粘接剂层的连接后的Tg高出5℃以上是理想的,而高出10℃以上是最理想的。
而且,第一粘接剂层与第二粘接剂层的厚度比为第一粘接剂层的厚度/第二粘接剂层的厚度=0.3至3.0,而理想的是在0.8至3.0。该范围以外的厚度经耐湿试验、冷热循环试验等各种可靠性试验后,有发生从基板脱落、剥离而无法获得优良的连接可靠性的倾向。
另外,在本发明中,使用上述二层构造的粘接剂层电连接相向的基板的电路电极时,理想的是将Tg较高的第一粘接剂层设置于相向的基板中的弹性率较高的基板侧。
上述热可塑性树脂或热固化性树脂均可作为本发明所使用的第一粘接剂层或第二粘接剂层,而从耐热性及可靠性的观点出发,理想的是使用热固化性树脂,尤其从低温硬化性的观点出发,使用(甲基)丙烯酸树脂、马来酰亚胺树脂、柠康酰亚胺树脂、降冰片烯酰亚胺树脂的自由基聚合系是理想的。
(甲基)丙烯酸树脂可由(甲基)丙烯酸酯类的自由基聚合而得,可以例举为(甲基)丙烯酸甲酯、(甲基)丙烯酸乙酯、(甲基)丙烯酸异丙酯、(甲基)丙烯酸异丁酯、乙二醇二(甲基)丙烯酸酯、二乙二醇二(甲基)丙烯酸酯、三羟甲基丙烷三(甲基)丙烯酸酯、四亚甲基二醇四(甲基)丙烯酸酯、2-羟基-1,3-二丙烯酰氧基丙烷、2,2-双[4-(丙烯酰氧基甲氧基)苯基]丙烷、2,2-双[4-(丙烯酰氧基乙氧基)苯基]丙烷、二环戊烯基(甲基)丙烯酸酯、三环癸烷基(甲基)丙烯酸酯、三(丙烯酰氧基乙基)异氰酸酯、氨酯(甲基)丙烯酸酯等,可以单独或组合二种以上使用。并且在不损害硬化性的范围内根据需要,加以使用氢醌、甲基醚氢醌等自由基聚合抑制剂1。
另外,在使用具有磷酸酯构造的自由基聚合性物质时,可提高对金属等无机物的粘接力。具有磷酸酯构造的自由基聚合性物质的使用量为,粘接剂组合物总量的0.1至10重量份,而理想的使用量是0.5至5重量份。具有磷酸酯构造的自由基聚合性物质可得自磷酸酐与2-羧基乙基(甲基)丙烯酸酯的反应产物。具体而言,有单(2-甲基丙烯酰氧基乙基)酸式磷酸盐、二(2-甲基丙烯酰氧基乙基)酸式磷酸盐等,可以单独或混合使用。
马来酰亚胺树脂是分子中具有至少一个马来酰亚胺基的树脂,例如苯基马来酰亚胺、1-甲基-2,4-双马来酰亚胺苯、N,N’-邻亚苯基双马来酰亚胺、N,N’-对亚甲基双马来酰亚胺、N,N’-4,4-亚联苯基双马来酰亚胺、N,N’-4,4-(3,3-二甲基亚联苯基)双马来酰亚胺、N,N’-4,4-(3,3-二甲基二苯基甲烷)双马来酰亚胺、N,N’-4,4-(3,3-二乙基二苯基甲烷)双马来酰亚胺、N,N’-4,4-二苯基甲烷双马来酰亚胺、N,N’-4,4-二苯基丙烷双马来酰亚胺、N,N’-4,4-二苯基醚双马来酰亚胺、N,N’-4,4-二苯基砜双马来酰亚胺、2,2-双(4-(4-马来酰亚胺)苯基)丙烷、2,2-双(3-二级丁基-3,4-(4-马来酰亚胺苯氧基)苯基)丙烷、1,1-双(4-(4-马来酰亚胺苯氧基)苯基)癸烷、4,4’-亚环己基双(1-(4-马来酰亚胺苯氧基)-2-环己基苯、2,2-双(4-(4-马来酰亚胺苯氧基)苯基)六氟丙烷等,可以单独或者二种以上混合使用。
柠康酰亚胺树脂是于分子中具有至少一个柠康酰亚胺基的柠康酰亚胺化合物的聚合物,柠康酰亚胺化合物是有例如苯基柠康酰亚胺、1-甲基-2,4-双柠康酰亚胺苯、N,N’-邻亚苯基双柠康酰亚胺、N,N’-对亚苯基双柠康酰亚胺、N,N’-4,4-亚联苯基双柠康酰亚胺、N,N’-4,4-(3,3-二甲基亚联苯基)双柠康酰亚胺、N,N’-4,4-(3,3-二甲基二苯基甲烷)双柠康酰亚胺、N,N’-4,4-(3,3-二乙基二苯基甲烷)双柠康酰亚胺、N,N’-4,4-二苯基甲烷双柠康酰亚胺、N,N’-4,4-二苯基丙烷双柠康酰亚胺、N,N’-4,4-二苯基醚双柠康酰亚胺、N,N’-4,4-二苯基砜双柠康酰亚胺、2,2-双(4-(4-柠康酰亚胺苯氧基)苯基)丙烷、2,2-双(3-二级丁基-3,4-(4-柠康酰亚胺苯氧基)苯基)丙烷、1,1-双(4,4(柠康酰亚胺苯氧基)苯基)癸烷、4,4’-亚环己基-双(1-(4-柠康酰亚胺苯氧基)苯氧基)-2-环己基苯、2,2-双(4-(4-柠康酰亚胺苯氧基)苯基)六氟丙烷等,可以单独或二种以上混合使用。
降冰片烯酰亚胺树脂是分子中具有至少一个降冰片烯酰亚胺基的降冰片烯酰亚胺化合物的聚合物,降冰片烯酰亚胺化合物是有例如苯基降冰片烯酰亚胺、1-甲基-2,4-双降冰片烯酰亚胺苯、N,N’-邻亚苯基双降冰片烯酰亚胺、N,N’-对亚苯基双降冰片烯酰亚胺、N,N’-4,4-亚联苯基双降冰片烯酰亚胺、N,N’-4,4-(3,3-二甲基亚联苯基)双降冰片烯酰亚胺、N,N’-4,4-(3,3-二甲基二苯基甲烷)双降冰片烯酰亚胺、N,N’-4,4-(3,3-二乙基二苯基甲烷)双降冰片烯酰亚胺、N,N’-4,4-二苯基甲烷双降冰片烯酰亚胺、N,N’-4,4-二苯基丙烷双降冰片烯酰亚胺、N,N’-4,4-二苯基醚双降冰片烯酰亚胺、N,N’-4,4-二苯基砜双降冰片烯酰亚胺、2,2-双(4-(4-降冰片烯酰亚胺苯氧基)苯基)丙烷、2,2-双(3-二级丁基-3,4-(4-降冰片烯酰亚胺苯氧基)苯基)丙烷、1,1-双(4-(4-降冰片烯酰亚胺苯氧基)苯基)癸烷、4,4’-亚环己基-双(1-(4-降冰片烯酰亚胺苯氧基)苯氧基)-2-环己基苯、2,2-双(4-(4-降冰片烯酰亚胺苯氧基)苯基)六氟丙烷等,可以单独或二种以上混合使用。
使用上述自由基聚合性化合物时,可使用聚合引发剂。作为聚合引发剂,只要是通过热或光产生自由基的化合物就没有特别的限制,例如有过氧化物、偶氮化合物等,可考虑目标的连接温度、连接时间、储存稳定性等而适当选择。从高反应性及储存稳定性的观点出发,以半衰期10小时的温度在40℃以上,且半衰期1分钟的温度在180℃以下的有机过氧化物是理想的,而以半衰期10小时的温度在50℃以上,且半衰期1分钟的温度在170℃以下的有机过氧化物是最理想的。连接时间为10秒时能够得到充分反应率的理想的硬化剂配比量是,粘接剂组合物总量的1至20重量%,而特别理想的是2至15重量%。本发明使用的有机过氧化物的具体化合物可选自二酰基过氧化物、过氧二碳酸酯、过氧酯类、过氧缩酮、二烷基过氧化物、氢过氧化物、硅烷基过氧化物等,其中特别理想的是过氧酯类、二烷基过氧化物、氢过氧化物、硅烷基过氧化物,是因为引发剂中的氯离子或有机酸在5,000ppm以下,加热分解后所产生的有机酸少且可抑制对电路构件的连接终端的腐蚀。
二酰基过氧化物类可列举异丁基过气化物、2,4-二氯苯甲酰基过氧化物、3,5,5-三甲基己酰基过氧化物、辛酰基过氧化物、月桂酰基过氧化物、硬脂酰基过氧化物、琥珀酰基过氧化物、苯甲酯基过氧化甲苯、苯甲酰基过氧化物等。
过氧二碳酸酯类可列举二正丙基过氧二碳酸酯、二异丙基过氧二碳酸酯、双(4-三级丁基环己基)过氧二碳酸酯、二-2-乙氧基甲氧基过氧二碳酸酯、二-(2-乙基己基过氧基)二碳酸酯、二甲氧基丁基过氧二碳酸酯、二(3-甲基-3-甲氧基丁基过氧基)二碳酸酯等。
过氧酯类可列举异丙苯基过氧化新癸酸酯、1,1,3,3-四甲基丁基过气化新癸酸酯、1-环己基-1-甲基乙基过氧化新癸酸酯、三级己基过氧化新癸酸酯、三级丁基过氧化三甲基醋酸酯、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-乙基己酸基过氧基)己烷、1-环己基-1-甲基乙基过氧化-2-乙基己酸酯、三级己基过氧化-2-乙基己酸酯、三级丁基过氧化-2-乙基己酸酯、三级丁基过氧化异丁酸酯、i,1-双(三级丁基过氧基)环己烷、三级己基过氧化异丙基单碳酸酯、三级丁基过氧化-3,5,5-三甲基己酸酯、三级丁基过氧化月挂酸酯、2,5-二甲基-2,5-二(间甲基苯甲酰基过氧基)己烷、三级丁基过氧化异丙基单碳酸酯、三级丁基过氧化-2-乙基己基单碳酸酯、三级己基过氧化苯甲酸酯、三级丁基过氧化醋酸酯等。
过氧缩酮类可列举1,1-双(三级己基过氧基)-3,3,5-三甲基环己烷、1,1-双(三级己基过氧基)环己烷、1,1-双(三级丁基过氧基)-3,3,5-三甲基环己烷、1,1-(三级丁基过氧基)环十二烷、2,2-双(三级丁基过氧基)癸烷等。
二烷基过氧化物气可列举α,α’-双(三级丁基过氧基)二异丙基苯、二异丙苯基过氧化物、2,5-甲-2,5-二(三级丁基过氧基)己烷、三级丁基异丙未基过氧化物等。
氢过氧化物类可列举二异丙基苯氢过氧化物、异丙苯氢过氧化物等。
硅烷基过氧化物类可列举三级丁基三甲基硅烷基过氧化物、双(三级丁基)二甲基硅烷基过氧化物、三级丁基三乙烯基硅烷基过氧化物、双(三级丁基)二乙烯基硅烷基过氧化物、三(三级丁基)二乙烯基过氧化物、三级丁基三烯丙基硅烷基过气化物、双(三级丁基)二烯丙基硅烷基过氧化物、三(三级丁基)烯丙基硅烷基过氧化物等。
为了抑制电路构件的连接终端的腐蚀或电路电极的腐蚀,理想的是在硬化剂中或上述有机过氧化物中所含有的氯离子或有机酸的量小于5,000ppm,并且加热分解后所产生的有机酸较少的有机过氧化物是更理想的。而且,为了提高所制作的电路连接材料的稳定性,理想的是在室温(25℃)、常压下打开放置24小时后重量保持率大于20重量%。使用时可以适当地混合上述有机过氧化物。
上述游离自由基产生剂可以单独或混合使用,也可与分解促进剂、抑制剂等混合使用。
并且,被聚氨酯系、聚酯系的高分子物质等包覆而被微胶囊化的固化剂,因使用时间得以延长所以是理想的。
热固化性树脂除了自由基聚合系,还有环氧树脂,环氧树脂有双酚A型环氧树脂、双酚F型环氧树脂、双酚S型环氧树脂、酚系清漆型环氧树脂、甲酚清漆型环氧树脂、双酚A清漆型环氧树脂、双酚F清漆型环氧树脂、脂环式环氧树脂、缩水甘油酯型环氧树脂、缩水甘油胺型环氧树脂、乙内酰脲型环氧树脂、异氰尿酸酯型环氧树脂、脂肪族链状环氧树脂等,上述环氧树脂也可被卤化,也可以被加氢。也可以组合二种以上的上述环氧树脂而使用。
另外,上述环氧树脂的固化剂有胺类、酚类、酸酐类、咪唑类、双氰胺类等通常的环氧树脂固化剂。另外,作为固化促进剂也可适当使用通常所用的三级胺类、有机磷系化合物。
而且,作为使环氧树脂反应的方法可以使用利用上述固化剂和锍盐、碘鎓盐等进行的阳离子聚合反应法。
为了赋予本发明的电路连接用粘接剂以成膜性、粘接性、固化时的应力松弛性,使用聚乙烯醇缩丁醛树脂、聚乙烯醇缩甲醛树脂、聚酯树脂、聚酰胺树脂、聚酰亚胺树脂、二甲苯树脂、苯氧基树脂、聚氨酯树脂、尿素树脂等高分子组分。上述高分子组分的重均分子量在10,000至10,000,000是理想的。并且,上述树脂也可以被改性为自由基聚合性官能基团,此时耐热性得到提高。另外,在上述树脂中含有羧基时,能够将其作为本发明中的含羧基的化合物而使用。高分子组分的配比量为粘接剂组合物总量的2至80重量%,理想的是5至70重量%,而10至60重量%是最理想的。如果小于2重量%,则应力的松弛或粘接力不充分,如果超过80重量%,则流动性变差。
本发明的电路连接用粘接剂中也可适当添加填充剂、软化剂、促进剂、老化防化剂、着色剂、阻燃剂、耦合剂。
本发明所用的电路连接用粘接剂是,即使不含导电粒子,连接时通过相向电极的直接接触也得以连接,但含有导电粒子时可得到更加稳定的连接。作为导电粒子可以使用Au、Ag、Ni、Cu、焊锡等金属粒子或在碳、玻璃、陶瓷、塑胶等非导电粒子表面上包覆Au、Ag、铂等贵金属类后的粒子。为了抑制金属离子表面的氧化,使用被贵金属类包覆后的金属粒子是理想的。上述导电粒子中,以塑胶作为核心、被Au、Ag等包覆的粒子或热熔融金属粒子通过连接时的加热加压变形,使接触面积增加并提高可靠性。贵金属类包覆层的厚度为100埃以上,理想的是在300埃以上,这时可得到良好的连接。而且,也可使用用绝缘性树脂包覆后的导电粒子作为上述导电离子。相对于粘接剂成分100体积%,导电粒子占0.1至30体积%,理想的是在0.1至10体积%范围内,根据用途适当配合。
而且,在本发明之1中,本发明的电路连接用粘接剂也可为固化物时的Tg(玻璃化转变温度)相差5℃以上的二种以上的层所构成的多层构造。
另外,在本发明之2中,在第一粘接剂层及第二粘接剂层的至少一层中含有酸当量在5至500(KOH毫克/克)的化合物是理想的。
使用本发明的电路连接用粘接剂进行粘接的基板是,只要形成电连接所需的电极的就可以,并没有特别的限制,有液晶显示器所使用的形成有薄膜透明电极(ITO)等电极的玻璃或塑胶基板,印刷电路板、陶瓷电路板、软性电路板、半导体硅芯片等,必要时可组合使用。
使用上述基板做连接时,将本发明之2的电路连接用粘接剂中的Tg较高的第一粘接剂层设置于弹性率较高的基板侧面是理想的。由此可更进一步减少脱落的发生。
连接时的条件并无特殊限制,连接温度为90至250℃,连接时间为1秒至10分钟,可依照使用的用途、粘接剂、基板等作适当选择,必要时也可进行后固化处理。并且,虽通过加热加压进行连接,而根据需要,使用热以外的其它能源,例如光、超声波、电磁波等也是可以的。
实施例
以下通过实施例更加具体地说明本发明,但本发明的范围并非仅限于该实施例。
按照以下配方分别进行混合,使用简易涂布机(测试器产业公司制)涂敷在厚度为50微米的单面经表面处理的PET(聚对苯二甲酸乙二醇酯)薄膜上,利用70℃,5分钟的热风干燥制作薄膜。
(氨酯丙烯酸酯的合成)
将重均分子量800的聚己内酯二醇400重量份,2-羟基丙基丙烯酸酯131重量份,作为催化剂的二丁基锡二月桂酯0.5重量份,及作为聚合抑制剂的氢醌单甲基醚1.0重量份,一边搅拌一边在50℃加热混合。接着滴入异佛尔酮二异氰酸酯222重量份,然后,一边搅拌一边升温至80℃进行氨酯化反应。确认反应率已达99%以上后,降低反应温度而得氨酯丙烯酸酯。
使用上述氨酯丙烯酸酯作为自由基聚合性物质。并且,使用羧酸改质的缩丁醛树脂(6000 EP;电气化学工业股份有限公司制商品名,酸当量250(KOH毫克/克))以及苯氧基树脂(PKHC;联合碳化公司制商名名,重均分子量45,000)作为薄膜形成材料。
使用三级己基过氧化-2-乙基己酸酯的50重量%DOP(酞酸二辛酯)溶液作为可通过加热产生游离自由基的固化剂。
使用以聚苯乙烯为核心,在其粒子表面设有厚度0.2微米的镍层,在该镍层的外侧设有厚度0.04微米的金层而制作的平均粒径4微米的导电粒子作为导电粒子。
实施例1
以固体成分重量比计,将经羧酸转化的缩丁醛树脂(以固体成分计)20克,苯氧基树脂(以固体成分计)30克,氨酯丙烯酸酯49克,磷酸酯型丙烯酸酯(共荣社油脂股份有限公司制,商品名P2M)1克,三级己基过氧化-2-乙基己酸酯5克(以DOP溶液计为10克)进行混合,再分散3体积%的导电粒子,涂布、干燥得到粘接剂层的厚度为8微米的电路连接材料。
(电路连接结构体的制作)
80℃,5秒,1MPa条件下,在形成有ITO电极的玻璃基板上临时连接做成1.5毫米宽长条的上述电路连接材料。将PET基材剥离,对准其安装TCP的电极,在150℃,20秒,4MPa条件下做正式连接。
实施例2
以固体成分重量比计,将羧酸转化的缩丁醛树脂(以固体成分计)30克,苯氧基树脂(以固体成分计)30克,氨酯丙烯酸酯39克,磷酸酯型丙烯酸酯(共荣社油脂股份有限公司制,商品名P2M)1克,三级己基过氧化-2-乙基己酸酯5克(以DOP溶液计为10克)进行混合,再分散混合3体积%的导电粒子,涂布、干燥得到粘接剂层的厚度为8微米的电路连接材料。
(电路连接结构体的制作)
80℃,5秒、1MPa条件下,在形成ITO电极的玻璃基板上临时连接做成1.5毫米宽长条的上述电路连接材料。将PET基材剥离,对准其安装TCP的电极,在150℃,20秒,4Mpa下做正式连接。
实施例3
以固体成分重量比计,将羧酸转化的缩丁醛树脂(以固体成分计)10克,苯氧基树脂(以固体成分计)35克,氨酯丙烯酸酯54克,磷酸酯型丙烯酸酯(共荣社油脂股份有限公司制,商品名P2M)1克,三级己基过氧化-2-乙基己酸酯5克(以DOP溶液计为10克)进行混合,再分散混合导电粒子3体积%,涂布、干燥得到粘接剂层的厚度为8微米的电路连接材料。
(电路连接结构体的制作)
将上述电路连接材料做成1.5毫米宽的长条,在形成ITO电极的玻璃基板上,80℃,5秒、1MPa条件下做临时连接。将PET基材剥离,对准其安装TCP的电极,在150℃,20秒,4Mpa下做正式连接。
比较例1
以固体成分重量比计,将苯氧基树脂(以固体成分计)45克,氨酯丙烯酸酯54克,磷酸酯型丙烯酸酯(共荣社油脂股份有限公司制,商品名P2M)1克,三级己基过氧化-2-乙基己酸酯5克(以DOP溶液计则为10克)进行混合,再分散混合导电粒子3体积%,得到粘接剂层的厚度为8微米的电路连接材料。
(电路连接结构体的制作)
将上述电路连接材料做成1.5毫米宽的长条,在形成ITO电极的玻璃基板上,80℃,5秒、1MPa条件下做临时连接。将PET基材剥离,对准其安装TCP的电极,在150℃,20秒,4Mpa下做正式连接。
(特性评估方法)
(1)连接电阻:使用atobandeisto(株)制的万用表TR 6848,以1毫安培的固定电流测定邻接电路间的电阻。
(2)粘接强度:依据J1S Z-0237进行,使用东洋精机制作所(株)制的STOROGRAPH E-S型,以90度剥离做测定。
(3)连接部分的观察:用金属显微镜观察连接部分有无剥离、气泡。
(4)可靠性评估:关于上述连接电阻,粘接力,在80℃、95%RH的条件进行高温高湿试验,240小时后取出,做项目(1)至(3)的试验。
其测定结果示于表1。
(表1)
项目 | 连接电阻(Ω) | 粘接力(N/m) | 连接部分的外观 | |||
初期 | 耐湿试验240小时后 | 初期 | 耐湿试验240小时后 | 初期 | 耐湿试验240小时后 | |
实施例1 | 2 | 2.2 | 1150 | 1000 | 良好 | 良好 |
实施例2 | 2.2 | 2.3 | 1290 | 1180 | 良好 | 良好 |
实施例3 | 2.1 | 2.4 | 1030 | 1030 | 良好 | 良好 |
比较例1 | 2.6 | 6.3 | 760 | 350 | 良好 | 发生脱落 |
本发明的实施例1至3均显示出良好的连接电阻、粘接力以及连接部分外观特性,耐湿试验后也显示良好的可靠性。相对于此、使用酸当量小于5(KOH毫克/克)的化合物的比较例中,粘接力的初期值低,而且,在耐湿试验后连接电阻变高,粘接力变低,发生剥落而连接可靠性差。
实施例4
(第一粘接剂层)
使用二羟甲基三环癸烷二丙烯酸酯以及上述氨酯丙烯酸酯作为自由基聚合性物质。
使用苯氧基树脂(PKHC;联合碳化公司制商品名,重均分子量45,000)作为薄膜形成材料。
使用三级己基过气化-2-乙基己酸酯的50重量%DOP(酞酸二辛酯)溶液作为通过加热产生游离自由基的固化剂。
在聚苯乙烯为核心的粒子表面设置厚度为0.2微米的镍层,在该镍层的外侧设置厚度0.04微米的金层,制作平均粒径4微米的导电粒子。
以固体成份的重量比计,混合苯氧基树脂(以固体成分计)50克,二羟甲基三环癸烷丙烯酸酯30克,氨酯丙烯酸酯19克,磷酸酯型丙烯酸酯(共荣社油脂股份有限公司制商品名;P2M)1克,三级己基过氧化-2-乙基己酸酯5克(以DOP溶液计则为10克),再分散混合3体积%的导电粒子,涂布、干燥得到粘接剂层厚度为8微米的电路连接材料(固化物的Tg为110℃)。
(第二粘接剂层)
使用氨酯丙烯酸酯做为自由基聚合性物质。
使用苯氧基树脂(PKHC;联合碳化公司制商品名,重均分子量45,000)作为薄膜形成材料。
使用三级己基过氧化-2-乙基己酸酯的50重量%DOP(酞酸二辛酯)溶液作为通过加热产生游离自由基的固化剂。
在聚苯乙烯为核心的粒子表面设置厚度0.2微米的镍层,在该镍层的外侧设置厚度0.04微米的金层,制作平均粒径4微米的导电粒子。
以固体成份的重量比计,混合苯氧基树脂(以固体成分计)50克,二羟甲基三环癸烷丙烯酸酯10公克,上述所合成的氨酯丙烯酸酯39克,磷酸酯型丙烯酸酯(共荣社油脂股份有限公司制商品名;P2M)1克,三级己基过氧化-2-乙基己酸酯5克(以DOP溶液计则为10克),再分散混合3体积%的导电粒子,涂布、干燥得粘接剂层厚度为18微米的电路连接材料(固化物的Tg为60℃)。
将第一粘接剂层和第二粘接剂层用辊筒积层机贴合成二层构造的电路连接用粘接剂。
实施例5
(第一粘接剂层)
除粘接剂层的厚度为12微米之外,与实施例4的第一粘接剂层同样方法获得电路连接材料(固化物的Tg为110℃)。
(第二粘接剂层)
除粘接剂层的厚度为15微米之外,与实施例4的第二粘接剂层同样方法获得电路连接材料(固化物的Tg为60℃)。
将第一粘接剂层及第二粘接剂层用辊筒积层机贴合成二层构造的电路连接用粘接剂。
实施例6
(第一粘接剂层)
除粘接剂层的厚度为18微米之外,以与实施例4的第一粘接剂层同样方法获得电路连接用材料(固化物的Tg为110℃)。
(第二粘接剂层)
除粘接剂层的厚度为14微米以外,以与实施例4的第二粘接剂层同样方法获得电路连接用材料(固化物的Tg为60℃)。
将第一粘接剂层及第二粘接剂层用辊筒积层机贴合成二层构造的电路连接用粘接剂。
实施例7
(第一粘接剂层)
使用苯氧基树脂(PKHC;联合碳化公司制商品名,重均分子量45,000)作为薄膜形成材料。
使用三级己基过氧基-2-乙基己酸酯的50重量%DOP(酞酸二辛酯)溶液作为可通过加热产生游离自由基的固化剂。
在以聚苯乙烯为核心的粒子表面设置厚度0.2微米的镍层,在该镍层的外侧设置厚度0.04微米的金层,制作平均粒径4微米的导电粒子。
以固体成分的重量比计:混合苯氧基树脂(以固体成分计)40克,二羟甲基三环癸烷二丙烯酸酯20克,氨酯丙烯酸酯39公克,磷酸酯型丙烯酸酯(共荣社油脂股份有限公司制商品名;P2M)1公克,三级己基过氧化-2-乙基己酸酯5公克(以DOP溶液计则为10公克),再分散混合3体积%的导电粒子,经涂布、干燥得到粘接剂层厚度为8微米的电路连接用材料(固化物的Tg为68℃)。
(第二粘接剂层)
利用苯氧基树脂(PKHC;联合碳化公司制商品名,重均分子量45,000)以及经羧酸转化的缩丁醛树脂(6000 EP;电气化学工业股份有限公司制商品名,酸当量250(KOH毫克/克))作为薄膜形成材料。
利用三级己基过氧化-2-乙基己酸酯的50重量%DOP(酞酸二辛酯)溶液作为可通过加热产生游离自由基的固化剂。
在以聚苯乙烯为核心的粒子表面设置厚度为0.2微米的镍层,然后在该镍层的外侧设置厚度为0.04微米的金层而制作平均粒径4微米的导电粒子。
以固体成分的重量比计,混合苯氧基树脂(以固体成分计)30克,经羧酸转化的缩丁醛树脂(以固体成分计)20克,二羟甲基三环癸烷二丙烯酸酯10克,上述所合成的氨酯丙烯酸酯39克,磷酸酯型丙烯酸酯(共荣社油脂股份有限公司制,商品名P2M)1克,三级己基过氧化-2-乙基己酸酯5克(以DOP溶液计为10克),再分散混合3体积%的导电粒子,经涂布、干燥得到粘接剂层厚度为18微米的电路连接材料(固化物的Tg为52℃)。
将第一粘接剂层及第二粘接剂层用辊筒积层机贴合成二层构造的电路连接用粘接剂。
比较例2
仅使用实施例4的第一粘接剂层,获得粘接剂层厚度为25微米的电路连接材料(固化物的Tg为110℃)。
比较例3
仅使用实施例4的第二粘接剂层,获得粘接剂层厚度为25微米的电路连接材料(固化物的Tg为60℃)。
(连接结构的制作)
将上述二层构造的电路连接用粘接剂做成1.5毫米宽的长条,在形成ITO电极的玻璃基板上(弹性率较高的基板侧),将Tg较高的第一粘接剂层设置于玻璃侧,在80℃,5秒,1MPa的条件下做临时连接。然后,将PET基材剥离,对准ITO的电极与TCP的电极的位置,在140℃,20秒,4MPa的条件下做正式连接。
另外,将实施例4的二层构造粘接剂中的Tg较低的第二粘接剂层设置于玻璃侧,在相同条件下进行连接,作为本发明的参考例。而且,对比较例2及3的电路连接用粘接剂也进行上述的操作。
(特性评估方法)
与实施例1至3及比较例1同样地进行。
特性评估结果示于表2。
(表2)
项目 | 连接电阻(Ω) | 粘接力(N/m) | 连接部分的外观 | |||
初期 | 耐湿试验240小时后 | 初期 | 耐湿试验240小时后 | 初期 | 耐湿试验240小时后 | |
实施例4 | 2.1 | 2.3 | 1200 | 1100 | 良好 | 良好 |
实施例5 | 2.2 | 2.5 | 1050 | 1000 | 良好 | 良好 |
实施例6 | 2.4 | 2.8 | 1250 | 1180 | 良好 | 良好 |
实施例7 | 2.5 | 2.9 | 1000 | 970 | 良好 | 良好 |
比较例2 | 2.2 | 2.2 | 1100 | 950 | 良好 | 发生脱落 |
比较例3 | 2.2 | 10 | 1250 | 450 | 良好 | 发生脱落 |
参考例 | 2.1 | 4.6 | 1100 | 650 | 良好 | 发生脱落 |
实施例4至7的任一例均具有连接电阻、粘著力,以及外观的良好结果,显示良好的连接可靠性。
相对于此,单层构造的比较例2及3中,Tg为110℃的比较例2,在耐湿试验后虽连接电阻没有发生变化而保持良好,但粘接力有所下降而发生脱落。并且,Tg较低为60℃的比较例3,在耐湿试验240小时后发现有连接电阻的上升,粘接力也降低。而且连接部分也发生脱落。
另一方面,若将Tg较低的第二粘接剂层设置于玻璃基板侧,则有发生脱落的情形,所以在本发明中理想的是将Tg较高的第一粘接剂层设置于玻璃基板侧。
根据本发明之1可提高初期及耐湿试验后的粘接力,并且可提供实现了连接温度的低温化和缩短连接时间的电路连接用粘接剂,以及使用该粘接剂的电路连接结构体。
并且,本发明之2的电路连接用粘接剂及使用该粘接剂的电路连接方法、电路连接结构体,提供可根据连接温度的低温化及连接时间的缩短化的要求,能在140℃以20秒作连接,且在连接后的耐湿试验中也没有发生剥离脱落,显示出优异连接可靠性的电路连接结构体。
Claims (19)
1.一种电路连接用粘接剂,是介于具有相向的电路电极的基板间,对具有相向的电路电极的基板加压,从而电连接加压方向的电极之间的电路连接用粘接剂,其特征为上述粘接剂中含有酸当量按KOH毫克/克计为5至500的化合物。
2.根据权利要求1所述的电路连接用粘接剂,其特征在于,酸当量按KOH毫克/克计为5至500的化合物是含有至少一个羧基的化合物。
3.根据权利要求1或2所述的电路连接用粘接剂,其特征在于,还含有自由基聚合性物质。
4.根据权利要求1或2所述的电路连接用粘接剂,其特征在于,还含有导电粒子。
5.根据权利要求3所述的电路连接用粘接剂,其特征在于,还含有导电粒子。
6.一种电路连接结构体,具有相向的电路电极的基板,电路连接用粘接剂介于具有相向的电路电极的基板之间,加压基板,从而电连接加压方向的电极,其特征在于,上述电路连接用粘接剂是权利要求1至4中的任一项所述的粘接剂。
7.一种电路连接用粘接剂,是介于具有相向的电路电极的基板间,对具有相向的电路电极的基板加压,从而电连接加压方向的电极之间的电路连接用粘接剂,其特征为上述粘接剂在粘接剂层的厚度方向具有第一粘接剂层及第二粘接剂层,而第一粘接剂层的加压连接后的玻璃化转变温度Tg高于第二粘接剂层的加压连接后的玻璃化转变温度Tg。
8.根据权利要求7所述的电路连接用粘接剂,其特征在于,第一粘接剂层的加压连接后的玻璃化转变温度Tg为50至200℃,第二粘接剂层的加压连接后的玻璃化转变温度Tg为40至100℃、且第1粘接剂层加压连接后的玻璃化转变温度Tg较第二粘接剂层的加压连接后玻璃化转变温度Tg高出5℃以上。
9.根据权利要求7所述的电路连接用粘接剂,其特征在于:在第一粘接剂层和第二粘接剂层中的至少一层中含有导电粒子。
10.根据权利要求8所述的电路连接用粘接剂,其特征在于:在第一粘接剂层和第二粘接剂层中的至少一层中含有导电粒子。
11.根据权利要求7至10任意一项所述的电路连接用粘接剂,其特征在于,第一粘接剂层和第二粘接剂层中的至少一层中含有自由基聚合性物质。
12.根据权利要求7至10任意一项所述的电路连接用粘接剂,其特征在于,第一粘接剂层与第二粘接剂层的厚度比为,第一粘接剂层的厚度/第二粘接剂层的厚度=0.3至3.0。
13.根据权利要求11所述的电路连接用粘接剂,其特征在于,第一粘接剂层与第二粘接剂层的厚度比为,第一粘接剂层的厚度/第二粘接剂层的厚度=O.3至3.0。
14.根据权利要求7至10任意一项所述的电路连接用粘接剂,其特征在于,第一粘接剂层及第二粘接剂层中的至少一层含有酸当量按KOH毫克/克计为5至500的化合物。
15.根据权利要求11所述的电路连接用粘接剂,其特征在于,第一粘接剂层及第二粘接剂层中的至少一层含有酸当量按KOH毫克/克计为5至500的化合物。
16.根据权利要求12所述的电路连接用粘接剂,其特征在于,第一粘接剂层及第二粘接剂层中的至少一层含有酸当量按KOH毫克/克计为5至500的化合物。
17.根据权利要求13所述的电路连接用粘接剂,其特征在于,第一粘接剂层及第二粘接剂层中的至少一层含有酸当量按KOH毫克/克计为5至500的化合物。
18.一种电路连接方法,是使电路连接用粘接剂介于具有相向的电路电极的基板之间,对具有相向的电路电极的基板加压,电连接加压方向的电极之间的方法,其特征在于,上述电路连接用粘接剂具有第一粘接剂层及第二粘接剂层,而第一粘接剂层的加压连接后的玻璃化转变温度Tg高于第二粘接剂层的加压连接后的玻璃化转变温度Tg,且加压连接后的玻璃化转变温度Tg较高的第一粘接剂层是设置于具有相向的电路电极的基板中弹性率较高的基板侧面而连接。
19.一种连接结构体,具有相向的电路电极的基板,电路连接用粘接剂介于具有相向的电路电极的基板之间,加压基板,电连接加压方向的电极,其特征为上述粘接剂具有第一粘接剂层及第二粘接剂层,而第一粘接剂层的加压连接后的玻璃化转变温度Tg高于第二粘接剂层的加压连接后的玻璃化转变温度Tg,且加压连接后的玻璃化转变温度Tg较高的第一粘接剂层是设置在具有相向的电路电极的基板中弹性率较高的基板侧面而连接。
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CN1425192A CN1425192A (zh) | 2003-06-18 |
CN1214455C true CN1214455C (zh) | 2005-08-10 |
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CNB018082556A Expired - Lifetime CN1214455C (zh) | 2000-04-25 | 2001-04-25 | 电路连接用粘接剂、使用其的电路连接方法及电路连接结构体 |
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US (3) | US7208105B2 (zh) |
JP (2) | JP3915512B2 (zh) |
KR (1) | KR100463558B1 (zh) |
CN (1) | CN1214455C (zh) |
AU (1) | AU2001252557A1 (zh) |
MY (1) | MY143567A (zh) |
TW (1) | TWI285216B (zh) |
WO (1) | WO2001082363A1 (zh) |
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CN102638944B (zh) * | 2007-04-19 | 2014-12-10 | 日立化成株式会社 | 电路连接用粘接薄膜、连接结构体以及其制造方法 |
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-
2001
- 2001-04-25 TW TW90109925A patent/TWI285216B/zh not_active IP Right Cessation
- 2001-04-25 CN CNB018082556A patent/CN1214455C/zh not_active Expired - Lifetime
- 2001-04-25 WO PCT/JP2001/003547 patent/WO2001082363A1/ja active IP Right Grant
- 2001-04-25 MY MYPI20011930A patent/MY143567A/en unknown
- 2001-04-25 JP JP2001579354A patent/JP3915512B2/ja not_active Expired - Fee Related
- 2001-04-25 US US10/258,548 patent/US7208105B2/en not_active Expired - Fee Related
- 2001-04-25 AU AU2001252557A patent/AU2001252557A1/en not_active Abandoned
- 2001-04-25 KR KR10-2002-7012143A patent/KR100463558B1/ko not_active IP Right Cessation
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2007
- 2007-03-21 US US11/723,644 patent/US20070166549A1/en not_active Abandoned
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2009
- 2009-05-21 JP JP2009122824A patent/JP2009182363A/ja active Pending
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Cited By (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN102638944B (zh) * | 2007-04-19 | 2014-12-10 | 日立化成株式会社 | 电路连接用粘接薄膜、连接结构体以及其制造方法 |
CN102768965A (zh) * | 2008-01-28 | 2012-11-07 | 瑞萨电子株式会社 | 半导体装置及其制造方法 |
CN102768965B (zh) * | 2008-01-28 | 2015-01-14 | 瑞萨电子株式会社 | 半导体装置及其制造方法 |
Also Published As
Publication number | Publication date |
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WO2001082363A1 (en) | 2001-11-01 |
CN1425192A (zh) | 2003-06-18 |
US20030141014A1 (en) | 2003-07-31 |
MY143567A (en) | 2011-05-31 |
AU2001252557A1 (en) | 2001-11-07 |
KR100463558B1 (ko) | 2004-12-29 |
US8029911B2 (en) | 2011-10-04 |
JP3915512B2 (ja) | 2007-05-16 |
JP2009182363A (ja) | 2009-08-13 |
US20070166549A1 (en) | 2007-07-19 |
KR20020084198A (ko) | 2002-11-04 |
US7208105B2 (en) | 2007-04-24 |
TWI285216B (en) | 2007-08-11 |
US20100294551A1 (en) | 2010-11-25 |
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