TWI534839B - Light reflective conductive particles, anisotropic conductive adhesives and light-emitting devices - Google Patents

Light reflective conductive particles, anisotropic conductive adhesives and light-emitting devices Download PDF

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Publication number
TWI534839B
TWI534839B TW103126553A TW103126553A TWI534839B TW I534839 B TWI534839 B TW I534839B TW 103126553 A TW103126553 A TW 103126553A TW 103126553 A TW103126553 A TW 103126553A TW I534839 B TWI534839 B TW I534839B
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Taiwan
Prior art keywords
light
particle
particles
reflective
anisotropic conductive
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Application number
TW103126553A
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English (en)
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TW201447922A (zh
Inventor
Hidetsugu Namiki
Shiyuki Kanisawa
Hideaki Umakoshi
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Dexerials Corp
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Publication of TW201447922A publication Critical patent/TW201447922A/zh
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Publication of TWI534839B publication Critical patent/TWI534839B/zh

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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
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J9/00—Adhesives characterised by their physical nature or the effects produced, e.g. glue sticks
    • C09J9/02—Electrically-conducting adhesives
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
    • C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
    • C08G59/40—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the curing agents used
    • C08G59/42—Polycarboxylic acids; Anhydrides, halides or low molecular weight esters thereof
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
    • C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L63/00—Compositions of epoxy resins; Compositions of derivatives of epoxy resins
    • C—CHEMISTRY; METALLURGY
    • 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
    • C09J11/00—Features of adhesives not provided for in group C09J9/00, e.g. additives
    • C09J11/02—Non-macromolecular additives
    • C09J11/04—Non-macromolecular additives inorganic
    • C—CHEMISTRY; METALLURGY
    • 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
    • C09J123/00—Adhesives based on homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Adhesives based on derivatives of such polymers
    • C09J123/02—Adhesives based on homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Adhesives based on derivatives of such polymers not modified by chemical after-treatment
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Description

光反射性導電粒子、異向性導電接著劑及發光裝置
本發明係關於一種用以將發光元件異向性導電連接於配線板之異向性導電接著劑用的光反射性導電粒子、含有其之異向性導電接著劑、及使用該接著劑將發光元件構裝於配線板而成之發光裝置。
使用發光二極體(LED，Light Emitting Diode)元件之發光裝置得到廣泛使用，舊式之發光裝置之結構係如圖4所示，用黏晶接著劑32將LED元件33接合於基板31上，並用金線37將其上面之p電極34及n電極35與基板31之連接端子36打線接合，將LED元件33整體用透明模樹脂38密封而成。然而，於圖4之發光裝置之情形時，存在以下問題：於LED元件33發出之光中，金線會吸收朝上面側出射之400~500nm之波長之光，又，朝下面側出射之光之一部分會被黏晶接著劑32吸收，而使LED元件33之發光效率降低。
因此，如圖5所示，提出將LED元件33覆晶構裝(專利文獻1)。於該覆晶構裝技術中，於p電極34與n電極35上分別形成有凸塊39，進而，於LED元件33之凸塊形成面上，以使p電極34與n電極35絕緣之方式設置光反射層40。並且，使用異向性導電膏41或異向性導電膜(未圖示)並使該等硬化來連接固定LED元件33與基板31。因此，於圖5之發光裝置中，朝LED元件33之上方出射之光不會被金線吸收，且朝下方出射之光之大部分由光反射層40反射而朝上方出射，因此發光效率(光取出效率)不會降低。
專利文獻1：日本特開平11-168235號公報
然而，於專利文獻1之技術中必須藉由金屬蒸鍍法於LED元件33上以使p電極34與n電極35絕緣之方式設置光反射層40，於製造上，存在無法避免成本增加之問題。
另一方面，於不設置光反射層40之情形時，亦存在以下問題：已硬化之異向性導電膏或異向性導電膜中之以金、鎳或銅包覆之導電粒子之表面呈茶色乃至暗茶色，又，分散有導電粒子之環氧樹脂黏合劑本身亦因其硬化所常用之咪唑系潛伏性硬化劑而呈茶色，從而難以提高發光元件發出之光的發光效率(光取出效率)，且無法使光之顏色(發光色)以其原本之顏色進行反射。
本發明之目的係解決以上先前技術之問題，並提供：於使用異向性導電接著劑將發光二極體(LED)元件等發光元件覆晶構裝於配線板來製造發光裝置時，即便不於LED元件上設置如會導致製造成本增加之光反射層，亦不會使發光效率降低，且不會於發光元件之發光色與反射光色之間產生色相差之光反射性導電粒子、含有其之異向性導電接著劑、及使用該接著劑將發光元件覆晶構裝於配線板而成之發光裝置。
本發明者於若使異向性導電接著劑本身具有光反射功能，則可使發光效率不降低之假設下，發現藉由在調配於異向性導電接著劑中之導電粒子之表面，設置由特定無機粒子所構成之白色~灰色之光反射層，則可使發光元件之發光效率不降低且於發光元件之發光色與導電粒子之反射光色之間不產生色相差，從而完成了本發明。
即，本發明提供一種光反射性導電粒子，其係用於用以將發光元件異向性導電連接於配線板之異向性導電接著劑用，且係由被金屬材料包覆之 核心粒子與於核心粒子表面由折射率為1.52以上之光反射性無機粒子形成之光反射層所構成。
又，本發明提供一種異向性導電接著劑，其係用以將發光元件異向性導電連接於配線板者，且係於熱硬化性樹脂組成物分散有上述光反射性導電粒子而成者，該熱硬化性樹脂組成物能提供對於波長380~780nm之可見光的光程長度1cm之透光率(JIS K7105)為80%以上之硬化物。
又，本發明提供一種發光裝置，其係經由上述異向性導電接著劑，將發光元件以覆晶方式構裝於配線板而成。
用以將發光元件異向性導電連接於配線板之異向性導電接著劑用之本發明之光反射性導電粒子，係由被金屬材料包覆之核心粒子與於核心粒子表面由折射率為1.52以上之光反射性無機粒子所形成之白色~灰色之光反射層所構成。又，本發明之異向性導電接著劑係於熱硬化性樹脂組成物分散有該光反射性導電粒子而成者，該熱硬化性樹脂組成物能提供對於波長380~780nm之可見光的光程長度1cm之透光率(JIS K7105)為80%以上的硬化物。因此，使用本發明之異向性導電接著層，將發光元件覆晶構裝於配線板所獲得之發光裝置即便使異向性導電接著劑硬化亦不產生著色，且所含有之光反射性導電粒子對可見光之反射特性之波長相依性較小，因此可使發光效率提高，且可使發光元件之發光色以其原本之顏色進行反射。
1‧‧‧核心粒子
2‧‧‧光反射性無機粒子
3‧‧‧光反射層
4‧‧‧熱塑性樹脂
10、20‧‧‧光反射性導電粒子
11‧‧‧熱硬化性樹脂組成物之硬化物
21、31‧‧‧基板
22、36‧‧‧連接端子
23、33‧‧‧LED元件
24、35‧‧‧n電極
25、34‧‧‧p電極
26、39‧‧‧凸塊
32‧‧‧黏晶接著劑
37‧‧‧金線
38‧‧‧透明模樹脂
40‧‧‧光反射層
41‧‧‧異向性導電膏
100‧‧‧異向性導電接著劑之硬化物
200‧‧‧發光裝置
圖1A係異向性導電接著劑用之本發明之光反射性導電粒子之剖面圖。
圖1B係異向性導電接著劑用之本發明之光反射性導電粒子之剖面圖。
圖2係本發明之發光裝置之剖面圖。
圖3係表示實施例1與比較例1之異向性導電接著劑之硬化物對波長之光反射率的圖。
圖4係先前之發光裝置之剖面圖。
圖5係先前之發光裝置之剖面圖。
一面參照圖式一面對本發明進行詳細說明。
圖1A、圖1B係異向性導電接著劑用之本發明之光反射性導電粒子10、20之剖面圖。首先，自圖1A之光反射性導電粒子開始說明。
光反射性導電粒子10由被金屬材料包覆之核心粒子1與於核心粒子1表面由折射率為1.52以上之光反射性無機粒子2所形成之光反射層3所構成。
折射率為1.52以上之光反射性無機粒子2係於太陽光下呈白色之無機粒子。因此，由該等形成之光反射層3呈白色~灰色。所謂呈白色~灰色，係指對可見光之反射特性之波長相依性較小，且易反射可見光。
較佳之光反射性無機粒子2可列舉選自氧化鈦(TiO2)粒子、氧化鋅(ZnO)粒子或氧化鋁(Al2O3)粒子之至少一種。另，於氧化鈦粒子、氧化鋅粒子或氧化鋁粒子中，當已硬化之異向性導電接著劑之熱硬化性樹脂之硬化物有發生光劣化的顧慮時，較佳為可使用對光劣化無觸媒性，且折射率亦較高之氧化鋅。
由於核心粒子1係一同參與異向性導電連接者，因此其表面由金屬材料構成。此處，表面由金屬材料包覆之態樣可列舉核心粒子1本身為金屬材料之態樣，或者樹脂粒子之表面由金屬材料包覆之態樣。
金屬材料可利用異向性導電連接用之先前導電粒子中所使用之金屬材料。例如，可列舉金、鎳、銅、銀、焊錫、鈀、鋁、該等之合金、該等之多層化物(例如，鍍鎳/金閃鍍敷物(gold flash plating))等。其中，由於金、鎳、銅使導電粒子呈茶色，因此與其他金屬材料相比更能展現本發明之效果。
另，當核心粒子1係由金屬材料包覆樹脂粒子而成者之情形時，樹脂粒子亦可利用先前以來用作為異向性導電連接用導電粒子之金屬包覆樹脂粒子之樹脂粒子部分。此種樹脂粒子可列舉苯乙烯系樹脂粒子、苯並胍胺(benzoguanamine)樹脂粒子、尼龍樹脂粒子等。以金屬材料包覆樹脂粒子之方法亦可採用先前公知之方法，可利用無電鍍法、電鍍法等。又，包覆之金屬材料之層厚為足以確保良好之連接可靠性之厚度，雖亦取決於樹脂粒子之粒徑或金屬之種類，但通常為0.1~3μm，較佳為0.1~1μm。
具有金屬材料表面之核心粒子1之粒徑若過小，則變得導通不良，若過大則有於圖案間發生短路之傾向，因此較佳為1~20μm，更佳為3~5μm。於此情形時，核心粒子1之形狀較佳為球形，亦可為薄片狀、橄欖球(rugby ball)狀。
關於由光反射性無機粒子2所形成之光反射層3之層厚，就與核心粒子1之粒徑之相對大小之觀點而言，相對於核心粒子1之粒徑，若過小則反射率會降低，若過大則有變得導通不良之傾向，因此較佳為0.5~50%，更佳為1~25%。
又，於光反射性導電粒子10中，關於構成光反射層3之光反射性無機粒子2之粒徑，若過小則難以產生光反射現象，若過大則有難以形成光反射層之傾向，因此較佳為0.02~4μm，更佳為0.1~1μm，特佳為0.2~0.5μm。於此情形時，就反射光的波長之觀點而言，為使應反射之光(即，發光元件發出之光)不會穿透，光反射性無機粒子2之粒徑較佳為該光之波長之50%以上。於此情形時，光反射性無機粒子2之形狀可列舉無定型、球狀、鱗片狀、針狀等，其中，就光擴散效果之方面而言較佳為球狀，就總反射效果之方面而言較佳為鱗片狀之形狀。
圖1A之光反射性導電粒子10可藉由公知之成膜技術(所謂機械融合 (Mechanofusion)法)來製造，即藉由使大小之粉末彼此發生物理性碰撞而於大粒徑粒子之表面形成由小粒徑粒子所構成之膜。於此情形時，光反射性無機粒子2係以陷入核心粒子1表面之金屬材料之方式而固定，另一方面，無機粒子彼此難以熔接固定，因此無機粒子之單層便構成光反射層3。因此，於圖1A之情形時，可認為光反射層3之層厚與光反射性無機粒子2之粒徑相等或略薄於光反射性無機粒子2之粒徑。
其次，對圖1B之光反射性導電粒子20進行說明。於該光反射性導電粒子20中，於光反射層3含有發揮出作為接著劑功能的熱塑性樹脂4，光反射性無機粒子2彼此亦由此熱塑性樹脂4所固定，因而光反射性無機粒子2多層化(例如多層化為2層或3層)，此點與圖1A之光反射性導電粒子10不同。藉由含有此種熱塑性樹脂4，光反射層3之機械強度會提高，並且變得難以發生無機粒子之脫落等。
圖1B之光反射性導電粒子20可藉由機械融合法進行製造。於此情形時，除光反射性無機粒子2與核心粒子1以外，再併用微粒子狀之熱塑性樹脂4即可。另，於藉由機械融合法製造圖1B之光反射性導電粒子20之情形時，亦同時製造圖1A之光反射性導電粒子10。
熱塑性樹脂4，為了減輕環境負荷而較佳為可使用無鹵素之熱塑性樹脂，例如，較佳為可使用聚乙烯、聚丙烯等聚烯烴或聚苯乙烯、丙烯酸樹脂等。
此種光反射性導電粒子20亦可藉由機械融合法進行製造。適用於機械融合法之熱塑性樹脂4之粒徑，若過小則作為接著劑之效果變小，若過大則變得難以附著於核心粒子1，因此較佳為0.02~4μm，更佳為0.1~1μm。又，關於此種熱塑性樹脂4之調配量，若過少則作為接著劑之效果較小，若過多則會生成不願見到之粒子凝聚體，因此相對於核心粒子1之100質量 份，較佳為0.2~500質量份，更佳為4~25質量份。
其次，對本發明之異向性導電接著劑進行說明。該異向性導電接著劑係於熱硬化性樹脂組成物分散有本發明之光反射性導電粒子而成者，可選取膏狀、膜狀等形態。
本發明之異向性導電接著劑中所使用之熱硬化性樹脂組成物，較佳為儘量使用無色透明者。原因在於，不會使異向性導電接著劑中之光反射性導電粒子之光反射效率降低，且在不改變入射光之光色下使其反射。此處，所謂無色透明，係指異向性導電接著劑之硬化物對於波長380~780nm之可見光的光程長度1cm之透光率(JIS K7105)為80%以上，較佳為90%以上。
於本發明之異向性導電接著劑中，光反射性導電粒子相對於熱硬化性樹脂組成物100質量份之調配量，若過少則變得導通不良，若過多則有於圖案間發生短路之傾向，因此較佳為1~100質量份，更佳為10~50質量份。
關於本發明之異向性導電接著劑之反射特性，為提高發光元件之發光效率，較理想的是異向性導電接著劑之100μm厚之硬化物對於波長450nm之光的反射率(JIS K7105)至少為15%。為達到此種反射率，只要對所使用之光反射性導電粒子之反射特性或調配量、熱硬化性樹脂組成物之調配組成等進行適當調整即可。通常，若增加反射特性良好之光反射性導電粒子之調配量，則有反射率亦增大之傾向。
又，亦可自折射率(JIS K7142)之觀點對異向性導電接著劑之反射特性進行評價。即，原因在於，若異向性導電接著劑之熱硬化性樹脂組成物與光反射性導電粒子之間的折射率之差過大，則光反射性導電粒子與包圍其之熱硬化性樹脂組成物之硬化物之界面中的光反射量會增大。具體而言，較理想的是熱硬化性樹脂組成物與光反射性無機粒子之間的折射率之差為0.02以上，較佳為0.3以上。另，通常，以環氧樹脂為主體之熱硬化性樹脂 組成物之折射率為約1.5。
構成本發明之異向性導電接著劑之熱硬化性樹脂組成物，可利用先前異向性導電接著劑或異向性導電膜中所使用者。一般而言，此種熱硬化性樹脂組成物係於絕緣性黏合樹脂中調配硬化劑而成者。絕緣性黏合樹脂，較佳為可列舉以脂環族環氧樹脂或雜環系環氧化合物或氫化環氧樹脂等為主成分之環氧系樹脂。
脂環族環氧化合物較佳為可列舉分子內具有2個以上環氧基者。該等既可為液態，亦可為固體狀。具體而言，可列舉縮水甘油基六氫雙酚A、3,4-環氧環己烯基甲基-3',4'-環氧環己烯甲酸酯等。其中，就可確保適宜於硬化物中構裝LED元件等之光透過性，且速硬化性亦優異之方面而言，較佳為可使用縮水甘油基六氫雙酚A、3,4-環氧環己烯基甲基-3',4'-環氧環己烯甲酸酯。
雜環系環氧化合物可列舉具有三口井環之環氧化合物，特佳為可列舉1,3,5-三(2,3-環氧丙基)-1,3,5-三嗪-2,4,6-(1H,3H,5H)-三酮。
氫化環氧化合物可使用上述脂環族環氧化合物或雜環系環氧化合物之氫化物，或其他公知之氫化環氧樹脂。
於本發明中，脂環族環氧化合物或雜環系環氧化合物或氫化環氧化合物既可單獨使用，亦可併用2種以上。又，除該等環氧化合物以外，只要不損及本發明之效果，亦可併用其他環氧化合物。例如可列舉：使雙酚A、雙酚F、雙酚S、四甲基雙酚A、二芳基雙酚A、氫醌、苯二酚、間苯二酚、甲酚、四溴雙酚A、三羥基聯苯、二苯甲酮、雙間苯二酚、雙酚六氟丙酮、四甲基雙酚A、四甲基雙酚F、三(羥苯基)甲烷、聯二甲苯酚、苯酚酚醛、甲酚酚醛等多酚與表氯醇反應所獲得之縮水甘油醚；使甘油、新戊二醇、乙二醇、丙二醇、丁二醇、己二醇、聚乙二醇、聚丙二醇等脂肪族多元醇 與表氯醇反應所獲得之聚縮水甘油醚；使如羥基苯甲酸、β-羥基萘甲酸之羥基羧酸與表氯醇反應所獲得之縮水甘油醚酯；由如鄰苯二甲酸、甲基鄰苯二甲酸、間苯二甲酸、對苯二甲酸、四氫鄰苯二甲酸、內亞甲基四氫鄰苯二甲酸、內亞甲基六氫鄰苯二甲酸、偏苯三甲酸、聚合脂肪酸之聚羧酸所獲得之聚縮水甘油酯；由胺基苯酚、胺基烷基苯酚所獲得之縮水甘油基胺基縮水甘油醚；由胺基苯甲酸所獲得之縮水甘油基胺基縮水甘油酯；由苯胺、甲苯胺、三溴苯胺、二甲苯二胺、二胺基環己烷、二胺基甲基環己烷、4,4'-二胺基二苯甲烷、4,4'-二胺基二苯基碸等所獲得之縮水甘油胺；環氧化聚烯烴等公知之環氧樹脂類。
硬化劑可使用酸酐、咪唑化合物、二氰等。其中，較佳為可使用不易使硬化物變色之酸酐，特佳為可使用脂環族酸酐系硬化劑。具體而言，較佳為可使用甲基六氫鄰苯二甲酸酐(MeHHPA)等。
於本發明之異向性導電接著劑之熱硬化性樹脂組成物中，使用脂環族環氧化合物與脂環族酸酐系硬化劑之情形時，關於各自之使用量，若脂環族酸酐系硬化劑過少則未硬化環氧化合物增多而產生硬化不良，若過多則有由於剩餘之硬化劑之影響而促進被黏附體材料腐蝕之傾向，因此相對於脂環族環氧化合物100質量份，較佳為以80~120質量份，更佳為以95~105質量份之比例使用脂環族酸酐系硬化劑。
本發明之異向性導電接著劑可藉由均勻地混合光反射性導電粒子與熱硬化性樹脂組成物而製造。又，於將異向性導電接著劑用作為異向性導電膜之情形時，只要進行以下處理即可：將該等與甲苯等溶劑一同分散混合，以達到所需之厚度之方式塗佈於經剝離處理之PET(polyethylene terephthalate，聚對苯二甲酸乙二酯)膜上，並於約80℃左右之溫度下進行乾燥。
其次，一面參照圖2一面對本發明之發光裝置進行說明。發光裝置200係於基板21上之連接端子22、與分別形成於作為發光元件之LED元件23之n電極24與p電極25之連接用凸塊26之間，塗佈上述本發明之異向性導電接著劑，因而覆晶構裝有基板21與LED元件23之發光裝置。此處，異向性導電接著劑之硬化物100係光反射性導電粒子10分散於熱硬化性樹脂組成物之硬化物11中而成者。另，視需要，亦可用透明模樹脂以覆蓋整個LED元件23之方式將其密封。
於如此所構成之發光裝置200中，於LED元件23發出之光中，朝基板21側發出之光由異向性導電接著劑之硬化物100中之光反射性導電粒子10反射，而自LED元件23之上面出射。因此，可防止發光效率之降低。
實施例
實施例1
(光反射性導電粒子之製成)
將平均粒徑0.5μm之氧化鈦粉末(KR-380，鈦工業(Titan Kogyo)(股))4質量份、以及外觀色為茶色之平均粒徑5μm之Au包覆樹脂導電粒子(對平均粒徑4.6μm之球狀丙烯酸樹脂粒子實施0.2μm厚之無電解鍍金而成之粒子：Bright 20GNB4.6EH，日本化學工業(股)20質量份，投入機械融合裝置(AMS-GMP，Hosokawa Micron(股))，並於旋轉速度1000rpm，旋轉時間20分鐘之條件下於導電粒子之表面形成由氧化鈦粒子所構成之約0.3μm厚之光反射層，藉此獲得實施例1之光反射性導電粒子。該光反射性導電粒子之外觀色為灰色。
(光反射率評價試驗)
使用真空消泡攪拌裝置將所獲得之光反射性導電粒子15質量份與折射率為約1.5之無色透明之熱硬化型環氧系黏合劑組成物(YX-8000， JER(股))100質量份均勻地混合，藉此獲得實施例1之異向性導電接著劑。
將所獲得之異向性導電接著劑以使乾燥厚度達到100μm之方式塗佈於陶瓷製之白色板上，並於200℃下加熱1分鐘，使其硬化。對於該硬化物，使用分光光度計(U3300，日立製作所(股))，測定對波長450nm之光之反射率(JIS K7105)。將所獲得之結果示於表1及圖3。
(電氣特性(導通可靠性、絕緣可靠性)評價試驗)
使用於光反射率評價試驗時所製備之異向性導電接著劑，於具有對50μm間距之銅配線實施Ni/Au(5.0μm厚/0.3μm厚)鍍敷處理而成之配線的環氧玻璃基板上，於200℃、60秒、1Kg/晶片之條件下覆晶構裝具有15μm高之金凸塊之6mm見方試驗用IC晶片(導體連接面積/導體-間隙=1600μm2/50μmP)，而獲得試驗用IC模組。
1.導通可靠性
對所獲得之試驗用IC模組交替進行加熱、冷卻至低溫(-40℃)與高溫(100℃)之溫度的溫度循環試驗(TCT，Temperature Cycle Test)(JIS C5030)，並藉由初始與500循環後之四端子法來測定電阻值。將電阻值未達1Ω之情形評價為「○」，將1Ω以上之情形評價為「×」。將所獲得之結果示於表1。
2.絕緣可靠性
對另外製成之試驗用IC模組進行於85℃、85%RH之環境下放置1000小時之老化試驗，並測定初始與1000小時後之電阻值。將電阻值為106Ω以上之情形評價為「○」，將未達106Ω之情形評價為「×」。將所獲得之結果示於表1。
實施例2
除使用平均粒徑5.0μm之Ni包覆樹脂導電粒子(52NR-4.6EH，日本化學工業(股))代替Au包覆樹脂導電粒子以外，以與實施例1同樣的方式， 獲得外觀色為灰色之光反射性導電粒子，進而獲得異向性導電接著劑。又，以與實施例1同樣的方式，進行光反射率評價試驗與電氣特性(導通可靠性、絕緣可靠性)評價試驗。將所獲得之結果示於表1。
實施例3
將平均粒徑0.5μm之氧化鈦粉末(KR-380，鈦工業(股))4質量份、作為接著劑粒子之平均粒徑0.2μm之聚苯乙烯(PS(polystyrene))粒子(Glossdell 204S，三井化學(股))3質量份、及平均粒徑5μm之導電粒子(對平均粒徑4.6μm之球狀丙烯酸樹脂粒子實施0.2μm厚之無電解鍍金而成之粒子：Bright 20GNB4.6EH，日本化學工業(股))20質量份，投入機械融合裝置(AMS-GMP，Hosokawa Micron(股))，且於旋轉速度1000rpm，旋轉時間20分鐘之條件下於導電粒子之表面形成由苯乙烯與氧化鈦粒子所構成之約1μm厚之光反射層，藉此獲得外觀色為灰色之光反射性導電粒子，進而獲得異向性導電接著劑。又，以與實施例1同樣的方式，進行光反射率評價試驗與電氣特性(導通可靠性、絕緣可靠性)評價試驗。將所獲得之結果示於表1。
實施例4
除使用平均粒徑5.0μm之Ni包覆樹脂導電粒子(52NR-4.6EH，日本化學工業(股))代替Au包覆樹脂導電粒子以外，以與實施例3同樣的方式，獲得外觀色為灰色之光反射性導電粒子，進而獲得異向性導電接著劑。又，進而以與實施例1同樣的方式，進行光反射率評價試驗與電氣特性(導通可靠性、絕緣可靠性)評價試驗。將所獲得之結果示於表1。
實施例5
除使用平均粒徑0.2μm之聚乙烯(PE(polyethylene))粒子(Chemipearl WF300，三井化學(股))，來代替平均粒徑0.2μm之聚苯乙烯粒子(Glossdell 204S，三井化學(股))以外，以與實施例3同樣的方式，獲得外觀色為灰色之 光反射性導電粒子，進而獲得異向性導電接著劑。又，以與實施例1同樣的方式，進行光反射率評價試驗與電氣特性(導通可靠性、絕緣可靠性)評價試驗。將所獲得之結果示於表1。
實施例6
除使用平均粒徑0.5μm之氧化鋅粉末(氧化鋅1種，Hakusuitech(股))代替平均粒徑0.5μm之氧化鈦粉末以外，以與實施例3同樣的方式，獲得外觀色為灰色之光反射性導電粒子，進而獲得異向性導電接著劑。又，以與實施例1同樣的方式，進行光反射率評價試驗與電氣特性(導通可靠性、絕緣可靠性)評價試驗。將所獲得之結果示於表1。
實施例7
除使用平均粒徑0.5μm之氧化鋁粉末(AE-2500SI，Admatechs(股))代替平均粒徑0.5μm之氧化鈦粉末以外，以與實施例3同樣的方式，獲得外觀色為灰色之光反射性導電粒子，進而獲得異向性導電接著劑。又，以與實施例1同樣的方式，進行光反射率評價試驗與電氣特性(導通可靠性、絕緣可靠性)評價試驗。將所獲得之結果示於表1。
實施例8
除使用平均粒徑0.5μm之碳酸鎂代替平均粒徑0.5μm之氧化鈦粉末以外，以與實施例3同樣的方式，獲得外觀色為灰色之光反射性導電粒子，進而獲得異向性導電接著劑。又，以與實施例1同樣的方式，進行光反射率評價試驗與電氣特性(導通可靠性、絕緣可靠性)評價試驗。將所獲得之結果示於表1。
實施例9
除使用平均粒徑0.2μm之氧化鈦粉末(JR405，Tayca(股))代替平均粒徑0.5μm之氧化鈦粉末以外，以與實施例3同樣的方式，獲得外觀色為灰色 之光反射性導電粒子，進而獲得異向性導電接著劑。又，以與實施例1同樣的方式，進行光反射率評價試驗與電氣特性(導通可靠性、絕緣可靠性)評價試驗。將所獲得之結果示於表1。
比較例1
使用外觀色為茶色之Au包覆樹脂導電粒子(對平均粒徑4.6μm之球狀丙烯酸樹脂粒子實施0.2μm厚之無電鍍金而成之粒子：Bright 20GNB4.6EH，日本化學工業(股))，以與實施例1同樣的方式，獲得異向性導電接著劑。又，以與實施例1同樣的方式，進行光反射率評價試驗與電氣特性(導通可靠性、絕緣可靠性)評價試驗。將所獲得之結果示於表1。亦將光反射率示於圖3。
比較例2
除使用外觀色為茶色之平均粒徑5.0μm之Ni包覆樹脂導電粒子(52NR-4.6EH，日本化學工業(股))代替Au包覆樹脂導電粒子以外，以與比較例1同樣的方式，獲得異向性導電接著劑。又，以與實施例1同樣的方式，進行光反射率評價試驗與電氣特性(導通可靠性、絕緣可靠性)評價試驗。將所獲得之結果示於表1。
比較例3
將平均粒徑0.2μm之聚苯乙烯系粒子(Glossdell 204S，三井化學(股))3質量份、以及平均粒徑5μm之導電粒子(對平均粒徑4.6μm之球狀丙烯酸樹脂粒子實施0.2μm厚之無電鍍金而成之粒子：Bright 20GNB4.6EH，日本化學工業(股))20質量份，投入機械融合裝置(AMS-GMP，Hosokawa Micron(股))，且於旋轉速度1000rpm，旋轉時間20分鐘之條件下於導電粒子之表面形成0.2μm厚之苯乙烯層，藉此獲得外觀色為茶色之樹脂包覆導電粒子，進而獲得異向性導電接著劑。又，以與實施例1同樣的方式， 進行光反射率評價試驗與電氣特性(導通可靠性、絕緣可靠性)評價試驗。將所獲得之結果示於表1。
比較例4
除使用平均粒徑0.5μm之氧化矽粉末(SEAHOSTER KEP-30，日本觸媒(股))代替平均粒徑0.5μm之氧化鈦粉末以外，以與實施例3同樣的方式，獲得外觀色為茶色之導電粒子，進而獲得異向性導電接著劑。又，以與實施例1同樣的方式，進行光反射率評價試驗與電氣特性(導通可靠性、絕緣可靠性)評價試驗。將所獲得之結果示於表1。
由表1可知以下結果：使用實施例1~9之光反射性導電粒子之異向性導電接著劑之光反射率均為30%以上，450nm之光之藍色以其原本之顏色進行反射。且導通可靠性及絕緣可靠性亦良好。
相對於此，於比較例1~3之情形時，由於未在導電粒子之表面設置光反射層，因此光反射率為10%左右，關於比較例1、2，自初始發生短路，於比較例3之情形時，於老化後發生短路，絕緣可靠性存在問題。於比較例4之情形時，由於使用氧化矽作為無機粒子，因此於形成無機粒子層後導電粒子之顏色亦呈茶色，且光反射率為10%左右。認為其原因在於，氧化矽與異向性導電接著劑之黏合劑組成物之間的折射率差未達0.02。
[產業上之可利用性]
本發明之光反射性導電粒子於使用異向性導電接著劑將發光二極體(LED)元件等發光元件覆晶構裝於配線板而製造發光裝置時，不需於發光元件上設置例如會導致製造成本增加之光反射層，而可使發光效率不降低，且可於發光元件之發光色與反射光色之間不產生色相差。由此，本發明之異向性導電接著劑於覆晶構裝LED元件時有用。
10‧‧‧光反射性導電粒子
11‧‧‧熱硬化性樹脂組成物之硬化物
21‧‧‧基板
22‧‧‧連接端子
23‧‧‧LED元件
24‧‧‧n電極
25‧‧‧p電極
26‧‧‧凸塊
100‧‧‧異向性導電接著劑之硬化物
200‧‧‧發光裝置

Claims (9)

  1. 一種光反射性導電粒子，係用於將發光元件異向性導電連接於配線板之異向性導電接著劑用的光反射性導電粒子，該光反射性導電粒子係由被金屬材料包覆之核心粒子，與於其表面由折射率為1.52以上之光反射性無機粒子形成之光反射層所構成，外觀顏色為灰色，該核心粒子之粒徑為1~20μm，光反射層之層厚為核心粒子徑的0.5~50%，該光反射性無機粒子係選自氧化鈦粒子、氧化鋅粒子或氧化鋁粒子之至少一種的無機粒子。
  2. 如申請專利範圍第1項之光反射性導電粒子，其中，包覆核心粒子之金屬材料為金、鎳或銅。
  3. 如申請專利範圍第1項之光反射性導電粒子，其中，核心粒子本身為金、鎳或銅之粒子。
  4. 如申請專利範圍第1項之光反射性導電粒子，其中，核心粒子係以金、鎳或銅包覆樹脂粒子者。
  5. 如申請專利範圍第2項之光反射性導電粒子，其中，核心粒子係以金、鎳或銅包覆樹脂粒子者。
  6. 如申請專利範圍第1至5項中任一項之光反射性導電粒子，其中，光反射層含有熱塑性樹脂。
  7. 如申請專利範圍第1至5項中任一項之光反射性導電粒子，其中，光反射層含有熱塑性樹脂。
  8. 如申請專利範圍第6項之光反射性導電粒子，其中，熱塑性樹脂為聚 烯烴。
  9. 如申請專利範圍第7項之光反射性導電粒子，其中，熱塑性樹脂為聚烯烴。
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