CN104364337A - 光反射性各向异性导电粘接剂及发光装置 - Google Patents
光反射性各向异性导电粘接剂及发光装置 Download PDFInfo
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- CN104364337A CN104364337A CN201380030476.3A CN201380030476A CN104364337A CN 104364337 A CN104364337 A CN 104364337A CN 201380030476 A CN201380030476 A CN 201380030476A CN 104364337 A CN104364337 A CN 104364337A
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Classifications
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- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- 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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- C09J183/00—Adhesives based on macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon, with or without sulfur, nitrogen, oxygen, or carbon only; Adhesives based on derivatives of such polymers
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- H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
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- H01L33/44—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the coatings, e.g. passivation layer or anti-reflective coating
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- H05K3/32—Assembling printed circuits with electric components, e.g. with resistor electrically connecting electric components or wires to printed circuits
- H05K3/321—Assembling printed circuits with electric components, e.g. with resistor electrically connecting electric components or wires to printed circuits by conductive adhesives
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- C08G77/388—Polysiloxanes modified by chemical after-treatment containing atoms other than carbon, hydrogen, oxygen or silicon containing nitrogen
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- H01L2224/45138—Material with a principal constituent of the material being a metal or a metalloid, e.g. boron (B), silicon (Si), germanium (Ge), arsenic (As), antimony (Sb), tellurium (Te) and polonium (Po), and alloys thereof the principal constituent melting at a temperature of greater than or equal to 950°C and less than 1550°C
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Abstract
一种为了将发光元件各向异性导电连接于布线板而使用的光反射性各向异性导电粘接剂,含有热固性树脂组合物、导电粒子和光反射性绝缘粒子。热固性树脂组合物含有:以式(1)表示的二缩水甘油基异氰尿酰基改性聚硅氧烷,和环氧树脂用固化剂。
Description
技术领域
本发明涉及一种为了将发光元件各向异性导电连接于布线板而使用的光反射性各向异性导电粘接剂、使用该粘接剂将发光元件安装于布线板而成的发光装置。
背景技术
使用发光二极管(LED)元件的发光装置得到广泛使用,如图3所示,老式的发光装置的结构为如下结构:将LED元件33用芯片接合(die bond)粘接剂32接合于基板31上,将其上面的p电极34和n电极35用金线37引线接合(wire bond)于基板31的连接端子36,将LED元件33整体用透明铸模树脂38密封。但是,在图3的发光装置的情况下,在LED元件33发射的光中,上面侧出射的400~500nm波长的光被金线吸收,而且在下面侧出射的光的一部分通过芯片接合粘接剂32吸收,有LED元件33的发光效率降低的问题。
因此,从提高LED元件的光反射所涉及的发光效率的角度出发,如图4所示,提出了倒装安装LED元件33 (专利文献1)。在该倒装安装技术中,在p电极34和n电极35上分别形成凸点39,进而在LED元件33的凸点形成面上设置光反射层40以使p电极34与n电极35绝缘。然后,使用各向异性导电糊41或各向异性导电膜(未图示),通过将它们固化从而使LED元件33与基板31连接固定。因此,在图4的发光装置中,由于向LED元件33的上方出射的光不被金线吸收,向下方出射的光的大部分由光反射层40反射而朝上方出射,所以发光效率(光取出效率)不降低。
另外,除了提高LED元件的光反射所涉及的发光效率的角度以外,从防止LED元件的安装中使用的各向异性导电糊或各向异性导电膜中的绝缘性树脂成分的由热或光导致的变色所伴随的LED元件的出射光颜色改变的角度出发,尝试在各向异性导电糊或各向异性导电膜中的绝缘性树脂成分中采用耐热性、耐光性优异的双液固化型甲基硅酮树脂或双液固化型苯基硅酮树脂。
现有技术文献
专利文献
专利文献1:日本特开平11-168235号公报。
发明内容
发明所要解决的课题
但是,在专利文献1的技术中,必须通过金属蒸镀法等在LED元件33上设置光反射层40以使p电极34与n电极35绝缘,在制备上有无法避免成本上升的问题;另一方面,在不设置光反射层40的情况下,固化的各向异性导电糊或各向异性导电膜中的用金、镍或铜被覆的导电粒子的表面呈现褐色乃至暗褐色,另外,分散有导电粒子的环氧树脂粘合剂本身也由于为了其固化而常用的咪唑类潜在性固化剂而呈现褐色,有难以提高发光元件发出的光的发光效率(光取出效率)的问题。
另外,当在各向异性导电糊或各向异性导电膜中的绝缘性树脂成分中采用双液固化型甲基硅酮树脂或双液固化型苯基硅酮树脂的情况下,虽然可抑制因热或光导致的绝缘性树脂成分的变色,但有LED元件相对于安装基板的剥离强度(晶片剪切强度:die shear strength)为不适于实际使用的水平的问题。
本发明的目的在于,解决以上以往的技术的问题,提供:一种各向异性导电粘接剂,其中在使用各向异性导电粘接剂将发光二极管(LED)元件等发光元件倒装安装于布线板从而制备发光装置时,即使在LED元件上不设置引起制备成本增大的光反射层,也可改善发光效率,并且,不仅难因热或光而变色,而且显示在实际使用上足够的晶片剪切强度;使用该粘接剂将发光元件倒装安装于布线板而成的发光装置。
解决课题的手段
本发明人发现,在若使各向异性导电粘接剂本身具有光反射功能,则可使发光效率不降低的假设下,通过在各向异性导电粘接剂中掺混光反射性绝缘粒子,可使发光元件的发光效率不降低。另外,本发明人发现,通过使用具有特定结构的二缩水甘油基异氰尿酰基(diglycidyl isocyanuryl)改性聚硅氧烷作为各向异性导电粘接剂的绝缘性粘接成分,可防止各向异性导电粘接剂因热或光而变色,并且,在实际使用上显示足够的晶片剪切强度。基于这些见解从而完成本发明。
即,本发明提供一种光反射性各向异性导电粘接剂,所述光反射性各向异性导电粘接剂是为了将发光元件各向异性导电连接于布线板而使用的光反射性各向异性导电粘接剂,其特征在于,含有热固性树脂组合物、导电粒子和光反射性绝缘粒子,热固性树脂组合物含有环氧树脂用固化剂和以式(1)表示的二缩水甘油基异氰尿酰基改性聚硅氧烷。
在式(1)中,R为烷基或芳基,n为1~40。
另外,作为该光反射性各向异性导电粘接剂的特别优选的实施方式,本发明提供一种光反射性各向异性导电粘接剂,其中,导电粒子为具有由金属材料被覆的芯粒子和在芯粒子表面上由选自氧化钛粒子、氮化硼粒子、氧化锌粒子或氧化铝粒子的至少一种无机粒子形成的光反射层的光反射性导电粒子。
另外,本发明提供经由上述光反射性各向异性导电粘接剂,将发光元件以倒装方式安装于布线板而成的发光装置。
发明的效果
为了将发光元件各向异性导电连接于布线板而使用的本发明的光反射性各向异性导电粘接剂含有作为粘合剂的热固性树脂组合物、光反射性绝缘粒子和导电粒子。该热固性树脂组合物含有用环氧树脂用固化剂固化的以式(1)表示的二缩水甘油基异氰尿酰基改性聚硅氧烷。该聚硅氧烷在其侧链上键合二缩水甘油基异氰尿酰基烷基。因此,可防止各向异性导电粘接剂因热或光而变色,并且,可实现在实际使用上足够的晶片剪切强度。
另外,由于本发明的光反射性各向异性导电粘接剂含有光反射性绝缘粒子,所以可反射光。特别是,在光反射性绝缘粒子为选自氧化钛粒子、氮化硼粒子、氧化锌粒子和氧化铝粒子的至少一种无机粒子、或在鳞片状或球状金属粒子的表面被覆有绝缘性树脂的树脂被覆金属粒子的情况下,由于粒子本身几乎为白色,所以对可见光的反射特性的波长依赖性小,因此,可提高发光效率,并且,可以原有的颜色反射发光元件的发光颜色。
另外,进而在使用具有由金属材料被覆的芯粒子与在其表面由氧化钛粒子、氮化硼粒子、氧化锌粒子或氧化铝粒子形成的白色~灰色的光反射层的光反射性导电粒子的情况下,由于该光反射性导电粒子本身呈现白色~灰色,所以对可见光的反射特性的波长依赖性小,因此,可进一步提高发光效率,并且,可以原有的颜色反射发光元件的发光颜色。
附图说明
[图1A] 图1A为本发明的光反射性各向异性导电粘接剂用的光反射性导电粒子的截面图
[图1B] 图1B为本发明的光反射性各向异性导电粘接剂用的光反射性导电粒子的截面图
[图2] 图2为本发明的发光装置的截面图
[图3] 图3为以往的发光装置的截面图
[图4] 图4为以往的发光装置的截面图。
具体实施方式
本发明为一种光反射性各向异性导电粘接剂,所述光反射性各向异性导电粘接剂是为了将发光元件各向异性导电连接于布线板而使用的光反射性各向异性导电粘接剂,含有热固性树脂组合物、导电粒子和光反射性绝缘粒子。首先,对作为粘合剂的热固性树脂组合物进行说明。
<热固性树脂组合物>
在本发明中,热固性树脂组合物含有以式(1)表示的二缩水甘油基异氰尿酰基改性聚硅氧烷和环氧树脂用固化剂。通过含有以式(1)表示的二缩水甘油基异氰尿酰基改性聚硅氧烷,可防止各向异性导电粘接剂因热或光而变色,并且,可实现在实际使用上足够的晶片剪切强度。
在式(1)中,R为碳原子数1~6的低级烷基等烷基,或碳环式芳族基、杂环式芳族基等芳基。作为烷基的优选的具体例,可列举出甲基、乙基、丙基、异丙基、丁基、异丁基,作为特别优选的烷基可列举出甲基。另外,作为芳基的优选的具体例,可列举出苯基。n为1~40的整数,优选为1~4的整数,更优选为1或2。
关于以式(1)表示的二缩水甘油基异氰尿酰基改性聚硅氧烷在热固性树脂组合物中的含量,若过少则有光反射性各向异性导电粘接剂的粘接性能降低的趋势,若过多则有使得未固化环氧成分量过多的趋势,所以优选为45~65质量%,更优选为50~60质量%。
另外,如以下反应式所示,以式(1)表示的二缩水甘油基异氰尿酰基改性聚硅氧烷可通过如下方法制备:在将式(a)的含氢聚硅氧烷和式(b)的1-烯丙基-3,5-二缩水甘油基异氰尿酸酯均匀混合后,在Karstedt催化剂(1,3-二乙烯基-1,1,3,3-四甲基二硅氧烷铂(0)络合物溶液)的存在下以室温~150℃加热。可通过常规方法(浓缩处理·柱处理)从反应混合物分离出式(1)的化合物。
除了式(1)的二缩水甘油基异氰尿酰基改性聚硅氧烷以外,热固性树脂组合物可在不损害发明的效果的范围内含有杂环类环氧化合物、脂环式环氧化合物或氢化环氧化合物等。
作为杂环类环氧化合物,可列举出具有三嗪环的环氧化合物,例如可列举出1,3,5-三(2,3-环氧丙基)-1,3,5-三嗪-2,4,6-(1H,3H,5H)-三酮(即三缩水甘油基异氰尿酸酯)。
作为脂环式环氧化合物,可优选列举出分子内具有2个以上环氧基的化合物。它们可为液态或固态。其中,从可确保固化物具有适合于LED的安装等的透光性、快速固化性也优异的方面出发,优选使用缩水甘油基六氢双酚A、3,4-环氧环己烯基甲基-3’,4’-环氧环己烯羧酸酯。
作为氢化环氧化合物,可使用上述杂环类环氧化合物或脂环式环氧化合物的氢化物,或其它公知的氢化环氧树脂。
相对于式(1)的二缩水甘油基异氰尿酰基改性聚硅氧烷,这些脂环式环氧化合物、杂环类环氧化合物或氢化环氧化合物可单独地并用或并用2种以上。另外,除了这些环氧化合物以外,只要不损害本发明的效果,可并用其它的环氧化合物。例如,可列举出使双酚A、双酚F、双酚S、四甲基双酚A、二芳基双酚A、氢醌、邻苯二酚、间苯二酚、甲酚、四溴双酚A、三羟基联苯、二苯甲酮、双间苯二酚(bisresorcinol)、双酚六氟丙酮、四甲基双酚A、四甲基双酚F、三(羟基苯基)甲烷、联二甲苯酚(bixylenol)、苯酚酚醛树脂(phenol novolac)、甲酚酚醛树脂(cresol novolac)等多元酚与表氯醇反应而得到的缩水甘油基醚,使甘油、新戊二醇、乙二醇、丙二醇、丁二醇、己二醇、聚乙二醇、聚丙二醇等脂族多元醇与表氯醇反应而得到的多缩水甘油基醚,使如对羟基苯甲酸、β-羟基萘甲酸之类的羟基羧酸与表氯醇反应而得到的缩水甘油基醚酯,由如邻苯二甲酸、甲基邻苯二甲酸、间苯二甲酸、对苯二甲酸、四氢邻苯二甲酸、桥亚甲基四氢邻苯二甲酸(endomethylene tetrahydrophthalic acid)、桥亚甲基六氢邻苯二甲酸(endomethylene hexahydrophthalic acid)、苯偏三酸、聚合脂肪酸之类的多聚羧酸得到的多缩水甘油酯,由氨基苯酚、氨基烷基苯酚得到的缩水甘油基氨基缩水甘油基醚,由氨基苯甲酸得到的缩水甘油基氨基缩水甘油酯,由苯胺、甲苯胺、三溴苯胺、苯二甲胺、二氨基环己烷、双氨基甲基环己烷、4,4’-二氨基二苯基甲烷、4,4’-二氨基二苯砜等得到的缩水甘油胺,环氧化聚烯烃等公知的环氧树脂类。
作为环氧树脂用固化剂,可使用公知的环氧树脂用固化剂。例如,可从胺类固化剂、聚酰胺类固化剂、酸酐类固化剂、咪唑类固化剂、聚硫醇类固化剂、多硫化物类固化剂、三氟化硼-胺络合物类固化剂、双氰胺、有机酰肼等中选择使用。其中,从透光性、耐热性等角度出发可优选使用酸酐类固化剂。
作为酸酐类固化剂,可列举出琥珀酸酐、邻苯二甲酸酐、马来酸酐、苯偏三酸酐、均苯四酸酐、六氢邻苯二甲酸酐、3-甲基-六氢邻苯二甲酸酐、4-甲基-六氢邻苯二甲酸酐、或4-甲基-六氢邻苯二甲酸酐与六氢邻苯二甲酸酐的混合物、四氢邻苯二甲酸酐、甲基-四氢邻苯二甲酸酐、纳迪克酸酐(nadic anhydride)、甲基纳迪克酸酐、降莰烷-2,3-二甲酸酐、甲基降莰烷-2,3-二甲酸酐、甲基环己烯二甲酸酐等。
相对于100质量份的以式(1)表示的二缩水甘油基异氰尿酰基改性聚硅氧烷,酸酐类固化剂等环氧树脂用固化剂在热固性树脂组合物中的掺混量若过少则有使得未固化环氧成分量过多的趋势,若过多则有因剩余的固化剂的影响而促进被附着物材料的腐蚀的趋势,所以优选为50~120质量份,更优选为60~100质量份。
为了顺利地且在短时间内完成固化反应,热固性树脂组合物可含有公知的固化促进剂。作为优选的固化促进剂,可列举出季鏻盐类固化促进剂或咪唑类固化促进剂。具体而言,可列举出季鏻的溴化物盐(“U-CAT5003”(商标),San-Apro Ltd.)、2-乙基-4-甲基咪唑等。特别是,作为酸酐类固化剂用的固化促进剂,可优选使用咪唑类固化促进剂。在该情况下,由于咪唑类固化促进剂的添加量若过少则有使得固化不充分的趋势,若过多则有对热·光的变色增大的趋势,所以相对于100质量份的酸酐类固化剂,咪唑类固化促进剂优选为0.20~2.00质量份,更优选为0.60~1.00质量份。
以上说明的热固性树脂组合物优选尽可能使用无色透明的组合物。其原因在于,不降低各向异性导电粘接剂中的光反射性导电粒子的光反射效率,并且,不改变入射光的光颜色地使其反射。此处,无色透明指各向异性导电粘接剂的固化物相对于波长为380~780nm的可见光,使得光路长度为1mm的透光率(JIS K7105)为80%以上、优选90%以上。
<光反射性绝缘粒子>
本发明的光反射性各向异性导电粘接剂含有的光反射性绝缘粒子用于将入射至各向异性导电粘接剂的光反射至外部。
需说明的是,具有光反射性的粒子包含金属粒子,将金属粒子被覆树脂的粒子,在自然光下为灰色~白色的金属氧化物、金属氮化物、金属硫化物等无机粒子,将树脂芯粒子用无机粒子被覆的粒子,不论粒子的材质的在其表面有凹凸的粒子。但是,在这些粒子中,由于要求显示绝缘性的关系,在本发明中可使用的光反射性绝缘粒子不包含未绝缘被覆的金属粒子。另外,在金属氧化物粒子中,不可使用如ITO那样具有导电性的粒子。另外,即使为显示光反射性且显示绝缘性的无机粒子,也不可使用如SiO2那样其折射率比使用的热固性树脂组合物的折射率低的粒子。
作为这样的光反射性绝缘粒子的优选的具体例,可列举出选自氧化钛(TiO2)粒子、氮化硼(BN)粒子、氧化锌(ZnO)粒子和氧化铝(Al2O3)粒子的至少一种无机粒子。其中,从高折射率的方面出发优选使用TiO2。
作为光反射性绝缘粒子的形状,可为球状、鳞片状、无定形状、针状等,但若考虑反射效率,则优选球状、鳞片状。另外,作为其大小,在为球状的情况下,由于有若过小则反射率变低、若过大则阻碍各向异性导电连接的趋势,所以优选为0.02~20μm,更优选为0.2~1μm;在为鳞片状的情况下,长径为优选0.1~100μm、更优选1~50μm,短径为优选0.01~10μm、更优选0.1~5μm,厚度为优选0.01~10μm、更优选0.1~5μm。
由无机粒子形成的光反射性绝缘粒子优选其折射率(JIS K7142)为优选比热固性树脂组合物的固化物的折射率(JIS K7142)大,更优选大至少0.02左右。其原因在于,若折射率差小则在它们的界面的反射效率降低。
作为光反射性绝缘粒子,可使用以上说明的无机粒子,或将鳞片状或球状金属粒子的表面用透明的绝缘性树脂被覆的树脂被覆金属粒子。作为金属粒子,可列举出镍、银、铝等。作为粒子的形状,可列举出无定形、球状、鳞片状、针状等,其中,从光扩散效果的方面出发优选球状,从全反射效果的方面出发优选鳞片状的形状。从光的反射率的方面出发特别优选的粒子为鳞片状银粒子。
虽然作为光反射性绝缘粒子的树脂被覆金属粒子的大小因形状而不同,但通常若过大,则有可能阻碍各向异性导电连接,若过小则使得光反射变难,所以优选在球状的情况下粒径为0.1~30μm、更优选0.2~10μm,在鳞片状的情况下,长径为优选0.1~100μm、更优选1~50μm且厚度为优选0.01~10μm、更优选0.1~5μm。此处,在绝缘被覆的情况下,光反射性绝缘粒子的大小为包含该绝缘被覆的大小。
作为这样的树脂被覆金属粒子中的有关树脂,可使用各种绝缘性树脂。从机械强度、透明性等方面出发可优选利用丙烯酸类树脂的固化物。优选地,可列举出在过氧化苯甲酰等有机过氧化物等自由基引发剂的存在下使甲基丙烯酸甲酯与甲基丙烯酸2-羟基乙酯自由基共聚而得的树脂。在该情况下,更优选用2,4-甲苯二异氰酸酯等异氰酸酯类交联剂进行交联。另外,作为金属粒子,优选预先用硅烷偶联剂将γ-环氧丙氧基或乙烯基等导入金属表面。
这样的树脂被覆金属粒子例如可通过如下方法制备:在甲苯等溶剂中投入金属粒子和硅烷偶联剂,于室温搅拌约1小时后,投入自由基单体和自由基聚合引发剂,并根据需要投入交联剂,一边加热至自由基聚合起始温度一边进行搅拌。
由于以上说明的光反射性绝缘粒子在光反射性各向异性导电粘接剂中的掺混量若过少则无法实现充分的光反射,另外,若过多则阻碍基于并用的导电粒子的连接,所以在光反射性各向异性导电粘接剂中含有优选为1~50体积%、更优选5~25体积%的光反射性绝缘粒子。
<导电粒子>
作为构成本发明的光反射性各向异性导电粘接剂的导电粒子,可利用在各向异性导电连接用的以往的导电粒子中使用的金属的粒子。例如,可列举出金、镍、铜、银、焊锡、钯、铝、它们的合金、它们的多层化物(例如镀镍/薄镀金物)等。其中,由于金、镍、铜使导电粒子为褐色,所以比其它的金属材料更能够享受到本发明的效果。
另外,作为导电粒子,可使用将树脂粒子用金属材料被覆的金属被覆树脂粒子。作为这样的树脂粒子,可列举出苯乙烯类树脂粒子、苯并胍胺树脂粒子、尼龙树脂粒子等。作为将树脂粒子用金属材料被覆的方法也可采用以往公知的方法,可利用非电解镀敷法、电解镀敷法等。另外,被覆的金属材料的层厚度为足以确保良好的连接可靠性的厚度,虽然也由树脂粒子的粒径、金属的种类决定,但通常为0.1~3μm。
另外,由于树脂粒子的粒径有若过小则产生导通不良、若过大则产生图案间短路的趋势,所以优选为1~20μm,更优选为3~10μm,特别优选为3~5μm。在该情况下,作为芯粒子1的形状优选球状,但也可为薄片状、橄榄球状。
优选的金属被覆树脂粒子为球状形状,由于其粒径若过大则使得连接可靠性降低,所以优选为1~20μm,更优选为3~10μm。
特别是,在本发明中,优选对如上所述的导电粒子赋予光反射性,制成光反射性导电粒子。图1A、图1B为这样的光反射性导电粒子10、20的截面图。首先,通过图1A的光反射性导电粒子进行说明。
光反射性导电粒子10由用金属材料被覆的芯粒子1和在其表面由选自氧化钛(TiO2)粒子、氮化硼(BN)粒子、氧化锌(ZnO)粒子或氧化铝(Al2O3)粒子的至少一种无机粒子2形成的光反射层3构成。氧化钛粒子、氮化硼粒子、氧化锌粒子或氧化铝粒子为在太阳光下呈现白色的无机粒子。因此,由它们形成的光反射层3呈现白色~灰色。呈现白色~灰色指对可见光的反射特性的波长依赖性小,并且,易反射可见光。
需说明的是,在氧化钛粒子、氮化硼粒子、氧化锌粒子或氧化铝粒子中,在担心固化的各向异性导电粘接剂的热固性树脂组合物的固化物发生光降解的情况下,可优选使用对光降解无催化性、折射率也高的氧化锌。
由于芯粒子1进行各向异性导电连接,所以用金属材料构成其表面。此处,作为用金属材料被覆表面的方式,如上所述,可列举出芯粒子1本身为金属材料的方式,或用金属材料被覆树脂粒子的表面的方式。
从与芯粒子1的粒径的相对大小的角度出发,相对于芯粒子1的粒径,由无机粒子2形成的光反射层3的层厚度若过小则反射率的降低变得明显,若过大则产生导通不良,所以优选为0.5~50%,更优选为1~25%。
另外,在光反射性导电粒子10中,由于构成光反射层3的无机粒子2的粒径有过小则使得难产生光反射现象、若过大则使得光反射层的形成变困难的趋势,所以优选为0.02~4μm,更优选为0.1~1μm,特别优选为0.2~0.5μm。在该情况下,若仅从光反射的光的波长的角度出发,则无机粒子2的粒径优选为应反射的光(即发光元件发出的光)的波长的50%以上,以使该光不透过。在该情况下,作为无机粒子2的形状可列举出无定形、球状、鳞片状、针状等,其中,从光扩散效果的方面出发优选球状,从全反射效果的方面出发优选鳞片状的形状。
图1A的光反射性导电粒子10可通过公知的成膜技术(所谓的机械熔合法:mechano-fusion)制备,其中,通过使大小粉末彼此物理性地碰撞而在大粒径粒子的表面形成由小粒径粒子制成的膜。在该情况下,无机粒子2以嵌入芯粒子1表面的金属材料中的方式固定,另一方面,由于难将无机粒子彼此熔接固定,所以无机粒子的单层构成光反射层3。因此,在图1A的情况下,光反射层3的层厚度可认为与无机粒子2的粒径相同乃至稍微变薄。
接着,对图1B的光反射性导电粒子20进行说明。在该光反射性导电粒子20中,光反射层3含有作为粘接剂起作用的热塑性树脂4,通过该热塑性树脂4也将无机粒子2彼此固定,无机粒子2多层化(例如多层化为2层或3层),在这一点上,与图1A的光反射性导电粒子10不同。通过含有这样的热塑性树脂4,使得光反射层3的机械强度提高,无机粒子的剥落等不易产生。
作为热塑性树脂4,为了实现环境低负担可优选使用无卤素的热塑性树脂,例如,可优选使用聚乙烯、聚丙烯等聚烯烃或聚苯乙烯、丙烯酸树脂等。
这样的光反射性导电粒子20也可通过机械熔合法来制备。由于应用于机械熔合法的热塑性树脂4的粒径若过小则粘接功能降低,若过大则变得难附着于芯粒子1,所以优选为0.02~4μm,更优选为0.1~1μm。另外,由于这样的热塑性树脂4的掺混量若过少则粘接功能降低,若过多则形成粒子的凝集体,所以相对于100质量份的无机粒子2,优选为0.2~500质量份,更优选为4~25质量份。
由于本发明的光反射性各向异性导电粘接剂中的光反射性导电粒子等导电粒子的掺混量若过少则有产生导通不良的趋势,若过多则有产生图案间短路的趋势,所以相对于100质量份的热固性树脂组合物,光反射性导电粒子等导电粒子的掺混量优选为1~100质量份,更优选为10~50质量份。
<光反射性各向异性导电粘接剂的制备>
本发明的光反射性各向异性导电粘接剂可通过将以上说明的光反射性绝缘粒子、导电粒子和热固性树脂组合物依据常规方法均匀地混合来制备。另外,在制成光反射性各向异性导电粘接膜的情况下,只要将它们与甲苯等溶剂一同分散混合,在经剥离处理的PET膜上涂布以便为所希望的厚度,于约80℃左右的温度干燥即可。
<光反射性各向异性导电粘接剂的反射特性>
为了提高发光元件的发光效率,关于本发明的光反射性各向异性导电粘接剂的反射特性,希望光反射性各向异性导电粘接剂的固化物对波长为450nm的光的反射率(JIS K7105)至少为30%。为了得到这样的反射率,只要适宜调整使用的光反射性绝缘粒子的反射特性或掺混量、热固性树脂组合物的掺混组成等即可。通常,若将反射特性良好的光反射性绝缘粒子的掺混量增量,则反射率也有增大的趋势。
另外,从折射率的角度出发也可评价光反射性各向异性导电粘接剂的反射特性。即,其原因在于,若该固化物的折射率比除去导电粒子和光反射性绝缘粒子的热固性树脂组合物的固化物的折射率大,则在光反射性绝缘粒子与包围它们的热固性树脂组合物的固化物之间的界面的光反射量增大。具体而言,希望光反射性粒子的折射率(JIS K7142)减去热固性树脂组合物的固化物的折射率(JIS K7142)的差为优选0.02以上、更优选0.2以上。需说明的是,通常,以环氧树脂为主体的热固性树脂组合物的折射率为约1.5。
<发光装置>
接着,在参照图2的同时对于本发明的发光装置进行说明。发光装置200为一种发光装置,其中,在基板21上的连接端子22与在作为发光元件的LED元件23的n电极24和p电极25上分别形成的连接用凸点26之间,涂布上述本发明的光反射性各向异性导电粘接剂,将基板21和LED元件23倒装安装。此处,光反射性各向异性导电粘接剂的固化物100中,光反射性绝缘粒子或导电粒子、优选光反射性导电粒子10分散于热固性树脂组合物的固化物11中。需说明的是,根据需要,可用透明铸模树脂以覆盖LED元件23整体的方式密封。另外,在LED元件23上也可与以往相同地设置光反射层。
在这样构成的发光装置200中,在LED元件23发出的光中,朝向基板21侧发出的光由光反射性各向异性导电粘接剂的固化物100中的光反射性绝缘粒子或光反射性导电粒子10反射,从LED元件23的上面出射。因此,可防止发光效率的降低。
本发明的发光装置200中的光反射性各向异性导电粘接剂以外的构成(LED元件23、凸点26、基板21、连接端子22等)可设为与以往的发光装置的构成相同。另外,本发明的发光装置200除了使用本发明的光反射性各向异性导电粘接剂以外,可利用以往的各向异性导电连接技术来制备。需说明的是,作为发光元件,除了LED元件以外,可在不损害本发明的效果的范围内应用公知的发光元件。
实施例
参考例(二缩水甘油基异氰尿酰基改性聚硅氧烷的制备)
在氮气流中,向具备回流冷却管和磁力搅拌器的100ml三颈瓶中投入28.12g (100.00mmol)的1-烯丙基-3,5-二缩水甘油基异氰尿酸酯(MADGIC,四国化成工业(株))和11.31g (40.02mmol)的1,3-双(三甲基甲硅烷氧基)-1,3-二甲基二硅氧烷(SIB1838.0,Gelest Inc.),将混合物于80℃搅拌至均匀地熔融。接着,向该熔融混合物中添加45.0μL的2% Karstedt催化剂溶液(二甲苯溶液),在搅拌的同时加热至变为120℃,从熔融混合物的温度达到120℃起,将该温度保持9小时,使1-烯丙基-3,5-二缩水甘油基异氰尿酸酯与1,3-双(三甲基甲硅烷氧基)-1,3-二甲基二硅氧烷反应。
在反应结束后,将反应混合物冷却,减压下(150℃/0.1kPa)蒸馏除去未反应单体,将残渣用柱色谱法(载体:硅胶,洗脱液:醋酸乙酯/己烷混合溶剂)处理,由此得到着色少的式(1a)的二缩水甘油基异氰尿酰基改性聚硅氧烷。
实施例1、比较例1-3
通过将表1所示的掺混组成的成分均匀地混合从而制备光反射性各向异性导电粘接剂。
需说明的是,在实施例1中,掺混环氧化合物和酸酐类固化剂使环氧基/酸酐的官能团数之比为1/1.1。另外,比较例2的各向异性导电粘接剂是在双液固化型二甲基硅酮树脂(IVS4742,Momentive Performance Materials Inc.)中掺混光反射性绝缘粒子和导电粒子而得,比较例3的各向异性导电粘接剂是在双液固化型苯基硅酮树脂(SCR-1012、信越化学工业(株))中掺混光反射性绝缘粒子和导电粒子而得。
(评价)
如以下说明那样测定得到的光反射性各向异性导电粘接剂的晶片剪切强度。另外,对于从光反射性各向异性导电粘接剂除去光反射性绝缘粒子和导电粒子的剩余的热固性树脂组合物,如以下说明那样,进行耐热试验和耐热光试验。将得到的结果示出于表2中。
<晶片剪切强度试验>
在具有形成有金凸点(高度为10μm,直径为80μm,间距为190μm)的厚度为10μm的全银电极的LED用玻璃环氧基板(特别定购品,关西电子工业(株)))上,涂布固化性树脂组合物使其直径为4mm,向此处放置0.3mm见方的倒装型LED元件(GM35R460G,昭和电工(株)),以使倒装型LED元件为外侧的方式将玻璃环氧基板放置于保持为80℃的热板上,加热2分钟而将LED元件临时固定于LED用玻璃环氧基板上。将临时固定有该LED元件的LED用玻璃环氧基板应用于热压接装置,在对LED元件施加80gf/chip的压力的同时于230℃进行15秒钟的热压接处理,由此制备在LED用玻璃环氧基板上安装有LED元件的LED装置。在使用实施例1或比较例1的光反射性各向异性导电粘接剂制备的LED装置的情况下,在热压接处理后进一步于260℃进行20秒的回流(reflow)处理。
对于这样制备的LED装置,测定晶片剪切强度(gf/chip)。在实际使用上,晶片剪切强度希望至少为200gf/chip,优选为250gf/chip以上。
<耐热试验>
用在四角配置有高度为1mm的垫片的2片铝平板(长度100mm×宽度50.0mm×厚度0.500mm)夹持热固性树脂组合物,对于实施例1和比较例1的热固性树脂组合物,首先于120℃加热30分钟,接着于140℃加热1小时,由此制备固化树脂片材。另外,对于比较例2和3的热固性树脂组合物,首先于80℃加热1小时,接着于150℃加热2小时,由此制备固化树脂片材。
将得到的固化树脂片材在设定为150℃的烘箱内放置1000小时,使用分光测色计(CM-3600d,Konica Minolta Inc.)测定放置前后的分光特性(L*、a*、b*),通过得到的测定值算出色差(ΔE)。在实际使用上,ΔE希望为35以下。
<耐热光试验>
制备与提供至耐热试验的固化树脂片材相同的固化树脂片材,将它于120℃的温度下在光强度设定为16mW/cm2的热光试验仪(Super Win Mini,Daypla Wintes Co., Ltd.;使用金属卤化物灯)内放置1000小时,将得到的固化树脂片材在设定为150℃的烘箱内放置1000小时,使用分光测色计(CM-3600d,Konica Minolta Inc.)测定放置前后的分光特性(L*、a*、b*),通过得到的测定值算出色差(ΔE)。在实际使用上,ΔE希望为20以下。
由表2可知,实施例1的光反射性各向异性导电粘接剂的晶片剪切强度、耐热试验和耐热光试验的结果均为在实际使用上优选的结果,而在比较例1的情况下,由于使用热固性环氧树脂组合物,所以对于晶片剪切强度虽然得到优选的结果,但由于未使用式(1a)的二缩水甘油基异氰尿酰基改性聚硅氧烷,所以对于耐热试验未得到可令人满意的结果。
需说明的是,对于比较例2和3,由于不仅未使用式(1a)的二缩水甘油基异氰尿酰基改性聚硅氧烷,而且未使用热固性环氧树脂组合物,所以晶片剪切强度非常低,无需进行耐热试验、耐热光试验。
产业上的可利用性
本发明的光反射性各向异性导电粘接剂可使得在使用各向异性导电粘接剂将发光二极管(LED)元件等发光元件倒装安装于布线板从而制备发光装置时,即使在发光元件上不设置引起制备成本增大的光反射层,也不降低发光效率。并且,晶片剪切强度也可维持高水平,耐热性、耐热光性也优异。因此,本发明的光反射性各向异性导电粘接剂在倒装安装LED元件时有用。
符号说明
1 芯粒子
2 无机粒子
3 光反射层
4 热塑性树脂
10、20 光反射性导电粒子
11 热固性树脂组合物的固化物
21 基板
22 连接端子
23 LED元件
24 n电极
25 p电极
26 凸点
100 光反射性各向异性导电粘接剂的固化物
200 发光装置。
Claims (14)
1. 一种光反射性各向异性导电粘接剂,所述光反射性各向异性导电粘接剂是为了将发光元件各向异性导电连接于布线板而使用的光反射性各向异性导电粘接剂,其特征在于,含有热固性树脂组合物、导电粒子和光反射性绝缘粒子,热固性树脂组合物含有环氧树脂用固化剂和以式(1)表示的二缩水甘油基异氰尿酰基改性聚硅氧烷:
式中,R为烷基或芳基,n为1~40的整数。
2. 权利要求1的光反射性各向异性导电粘接剂,其中,R为甲基,n为1~40的整数。
3. 权利要求1或2的光反射性各向异性导电粘接剂,其中,相对于式(1)的二缩水甘油基异氰尿酰基改性聚硅氧烷100质量份,热固性树脂组合物含有50~120质量份的环氧树脂用固化剂。
4. 权利要求1~3中任一项的光反射性各向异性导电粘接剂,其中,环氧树脂用固化剂为酸酐类固化剂。
5. 权利要求4的光反射性各向异性导电粘接剂,其中,热固性树脂组合物进一步含有咪唑类固化促进剂。
6. 权利要求5的光反射性各向异性导电粘接剂,其中,相对于酸酐类固化剂100质量份,热固性树脂组合物含有0.20~2.00质量份的咪唑类固化促进剂。
7. 权利要求1~6中任一项的光反射性各向异性导电粘接剂,其中,光反射性绝缘粒子为选自氧化钛粒子、氮化硼粒子、氧化锌粒子和氧化铝粒子的至少一种无机粒子。
8. 权利要求1~7中任一项的光反射性各向异性导电粘接剂,其中,光反射性绝缘粒子的折射率(JIS K7142)比热固性树脂组合物的固化物的折射率(JIS K7142)大。
9. 权利要求1~8中任一项的光反射性各向异性导电粘接剂,其中,光反射性绝缘粒子为将鳞片状或球状金属粒子的表面用绝缘性树脂被覆的树脂被覆金属粒子。
10. 权利要求1~9中任一项的光反射性各向异性导电粘接剂,其中,光反射性各向异性导电粘接剂含有1~50体积%的光反射性绝缘粒子。
11. 权利要求1~10中任一项的光反射性各向异性导电粘接剂,其中,导电粒子为具有由金属材料被覆的芯粒子和在芯粒子表面上的光反射层的光反射性导电粒子,所述光反射层由选自氧化钛粒子、氮化硼粒子、氧化锌粒子或氧化铝粒子的至少一种无机粒子形成。
12. 权利要求11的光反射性各向异性导电粘接剂,其中,相对于100质量份的热固性树脂组合物,光反射性导电粒子的掺混量为1~100质量份。
13. 经由权利要求1~12中任一项的光反射性各向异性导电粘接剂,将发光元件以倒装方式安装于布线板而成的发光装置。
14. 权利要求13的发光装置,其中,发光元件为发光二极管。
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