TWI352109B - - Google Patents

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Publication number
TWI352109B
TWI352109B TW096135750A TW96135750A TWI352109B TW I352109 B TWI352109 B TW I352109B TW 096135750 A TW096135750 A TW 096135750A TW 96135750 A TW96135750 A TW 96135750A TW I352109 B TWI352109 B TW I352109B
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TW
Taiwan
Prior art keywords
circuit
particles
conductive
substrate
polymer electrolyte
Prior art date
Application number
TW096135750A
Other languages
English (en)
Other versions
TW200829677A (en
Inventor
Nobuaki Takane
Original Assignee
Hitachi Chemical Co Ltd
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Publication date
Application filed by Hitachi Chemical Co Ltd filed Critical Hitachi Chemical Co Ltd
Publication of TW200829677A publication Critical patent/TW200829677A/zh
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Publication of TWI352109B publication Critical patent/TWI352109B/zh

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    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K3/00—Apparatus or processes for manufacturing printed circuits
    • H05K3/30—Assembling printed circuits with electric components, e.g. with resistor
    • 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
    • H05K3/323—Assembling printed circuits with electric components, e.g. with resistor electrically connecting electric components or wires to printed circuits by conductive adhesives by applying an anisotropic conductive adhesive layer over an array of pads
    • 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
    • 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
    • C09J9/00—Adhesives characterised by their physical nature or the effects produced, e.g. glue sticks
    • C09J9/02—Electrically-conducting adhesives
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    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
    • H01B1/20—Conductive material dispersed in non-conductive organic material
    • H01B1/22—Conductive material dispersed in non-conductive organic material the conductive material comprising metals or alloys
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Description

1352109 九、發明說明 【發明所屬之技術領域】 本發明係關於各向異導電性黏著劑組成物、 電性薄膜、電路構件之連接構造、及被覆粒子之 ;更詳細而言，係關於連接電路基板彼此或1C 電子零件與配線基板所使用的各向異導電性黏著 、使用其之各向異導電性薄膜、電路構件之連接 被覆粒子之製造方法。 【先前技術】 使電路基板彼此或1C晶片等之電子零件與 進行電連接時，使用將導電粒子分散於黏著劑組 各向異導電性黏著劑組成物，亦即，將此各向異 著劑組成物，配置於如上述的互相對峙之電路構 間，藉由加熱及加壓連接電極彼此，使加壓方向 性，可進行對向的電極間的電連接與電路構件彼 (例如參考專利文獻1及2 )。 液晶顯示用玻璃嵌板（glass panel )，係藉丨 C h i ρ · Ο η - G1 a s s )實裝或 COF ( Chip-On-Flex )實 液晶驅動用IC被實裝。COG實裝，係使用含有 之各向異導電性黏著劑組成物直接將液晶驅動用 於玻璃嵌板上；COF實裝，係將液晶驅動用1C 有金屬配線之柔性帶（FLEXIBLE TAPE)，使用 粒子之各向異導電性黏著劑組成物將此等黏合於 各向異導 製造方法 晶片等之 劑組成物 構造、及 電路基板 成物中之 導電性黏 件的電極 具有導電 此之固定 & COG ( 裝，而使 導電粒子 1C黏合 黏合於具 含有導電 玻璃嵌板 -4- 1352109 但近年來，隨著液晶顯示的高精細化，而1C的電路 電極之金凸塊的窄間距化、窄面積化，其他的電子零件亦 朝向高精細化發展，因此，會有因爲各向異導電性黏著劑 組成物中的導電粒子流出至相鄰的電路電極間，而產生短 路之虞。 解決此問題之方法，已開發了藉由在電路連接構件的 至少單面上形成絕緣性的黏著層，以防止COG實裝或 COF實裝之黏合品質的降低之方法（例如參考專利文獻3 )、用絕緣性的皮膜被覆導電粒子的全部表面之方法（例 如參考專利文獻4)，此外，亦提議使用被覆導電粒子表 面的一部份被絶緣性微粒子被覆的被覆粒子之方法（例如 參考專利文獻5及6 )，又，如此的絶緣性被覆之方法， 提議交互層合聚陰離子薄膜與聚陽離子薄膜的高分子電解 質薄膜之方法（例如參考專利文獻7 )。 專利文獻1 :特許第3 5 8 1 6 1 8號公報 專利文獻2:特許第3679618號公報 專利文獻3 :特開平8 -27 93 7 1號公報 專利文獻4 :特許第2794009號公報 專利文獻5:特開2005-197089號公報 專利文獻6:國際公開W02003/025955號文獻 專利文獻7:特開2003-317827號公報 【發明內容】
-5- k ^ J 1352109 〔發明所欲解決之課題〕 惟，上述專利文獻3所記載之於電路連接構件的單面 上形成絕緣性的黏著層之方法，例如凸塊面積爲3 00 0 " m2以下，爲了得到安定的連接電阻而增加導電粒子數時， 相鄰的電路電極間的絕緣性尙有改良的餘地；此外，上述 專利文獻4所記載之用絕緣性的皮膜被覆導電粒子的全部 表面之方法，會有對向之電路電極間的連接電阻上昇，無 法得到安定的電阻之問題；而且，上述專利文獻5所記載 之使用導電粒子表面的一部份被絕緣性微粒子被覆之被覆 粒子時，會殘留重複進行信賴性試驗則電阻上昇之問題； 此外，上述專利文獻6所記載之被覆粒子的形成方法，會 有必需要有於導電粒子及絕緣粒子上導入官能基之製程， 以及因爲各官能基之間的相互作用弱，故絕緣粒子不易凝 聚在導電粒子上，產率變差，且絕緣性產生偏差之課題； 另外，上述專利文獻7所記載之被覆粒子的形成方法，雖 然可無缺陷且均勻的被覆導電粒子的表面，但會有對向之 電路電極間的連接電阻上昇，無法得到安定的電阻之問題 〇 本發明係鑑於上述先前技術所具有的課題而完成之發 明，目的在於提供可提供即使連接間距變爲窄間距時，亦 可充分的抑制因爲分散的被覆粒子凝聚而於相鄰電路電極 間發生短路，可得到優異的長期連接信賴性之各向異導電 性黏著劑組成物、使用其之各向異導電性薄膜、電路構件 之連接構造、及被覆粒子之製造方法。 -6- 1352109 〔用以解決課題之手段〕 爲了解決上述問題，本發明係提供一種各向異導 黏著劑組成物，其係用於使第一基板的主面上形成第 路電極之第一電路構件、與第二基板的主面上形成第 路電極之第二電路構件，在該第一電路電極與該第二 電極爲對向配置狀態下連接之各向異導電性黏著劑組 ，其特徵係含有黏著劑、及導電粒子表面的至少一部 含有高分子電解質與無機氧化物微粒子的絕緣性材料 之被覆粒子。 依據本發明的各向異導電性黏著劑組成物，因爲 上述的被覆粒子取代一般的導電粒子作爲導電性材料 使連接間距變成窄間距時（例如相鄰的電極間之間距: /zm以下的窄間距時）被覆粒子凝聚，亦可藉由含有 子電解質與無機氧化物微粒子之絕緣性材料所成的皮 保持導電粒子間的絕緣性，且可充分的抑制電極間短 發生。此外，於對向的電極間，藉由連接電路構件彼 之壓力而可得到加壓方向的導電性，確保電連接。使 機氧化物微粒子作爲絕緣性材料，則因爲連接步驟的 、加熱所造成的變形及回復的情況少，故連接部份的 上昇或之後的電阻値的上昇受到抑制，而可得到優異 期連接信賴性。又，因爲絕緣性粒子含有高分子電解 而不需要在導電粒子及絕緣粒子表面上導入官能基之 ，故可在產率佳的狀況下製造，而且絕緣性不易產生 電性 -電 二電 電路 成物 份被 被覆 使用 ，即 ^ 15 高分 膜而 路的 此時 用無 加壓 電阻 的長 質， 製程 偏差 V % \ ^ J. 1352109 此外，本發明的各向異導電性黏著劑組成物中，其中 該被覆粒子係該導電粒子表面的至少一部份上，該高分子 電解質與該無機氧化物微粒子交互的靜電吸附而成者較佳 。因爲藉由導電粒子的表面上吸附高分子電解質，在高分 子電解質與無機氧化物微粒之靜電引力產生作用，可使無 機氧化物微粒子選擇性的吸附於導電粒子表面，認爲此乃 因爲無機氧化物微粒子表面上具有羥基等之極性基。 再者，本發明的各向異導電性黏著劑組成物，其中該 無機氧化物微粒子係由含有選自矽、鋁、锆、鈦、鈮、鋅 、錫、铈及鎂所成群的至少一種元素的氧化物所成者較佳 ，藉此，使其作爲一種對於化學、熱爲安定的絕緣性粒子 進行作用。 此外，本發明的各向異導電性黏著劑組成物，其中該 無機氧化物微粒子的平均粒徑爲20〜500nm的範圍內較佳 。藉由使無機氧化物微粒子的平均粒徑位於上述範圍內， 可充分確保相鄰電極間的絕緣性，同時可充分確保連接時 的加壓方向的導電性。 而且，本發明的各向異導電性黏著劑組成物，該高分 子電解質係不含鹼金屬離子、鹼土類金屬離子及鹵化物離 子者較佳，藉此，可充分的抑制電致遷移或腐蝕的發生。 本發明更提供一種各向異導電性薄膜，其係將上述本 發明的各向異導電性黏著劑組成物形成薄膜而成。 依據該相關的各向異導電性薄膜，因爲使用了上述本 -8- 1352109 發明的各向異導電性黏著劑組成物，故即使連接間距變成 窄間距時，亦可充分的抑制因爲分散的導電粒子凝聚而於 相鄰電路電極間發生短路，可得到優異的長期連接信賴性 ，此外，該相關的各向異導電性薄膜，因爲是薄膜狀故操 作容易。 本發明更提供一種電路構件之連接構造，其特徵係第 —基板的主面上形成第一電路電極之第一電路構件、與第 二基板的主面上形成第二電路電極之第二電路構件，藉由 被設置在該第一及第二電路構件之間之本發明的各向異導 電性黏著劑組成物的硬化物所成的電路連接構件，使該第 一電路電極與該第二電路電極對峙的同時進行電連接。 該相關的電路構件之連接構造，因爲電路連接構件由 上述本發明的各向異導電性黏著劑組成物的硬化物所成， 故即使連接間距變爲窄間距時，可充分的抑制因爲分散的 被覆粒子凝聚而於相鄰電路電極間發生短路，可得到優異 的長期連接信賴性。 在此，在上述第一電路構件中，該第一基板爲玻璃基 板，而且該第一電路電極爲金屬電極電路，該第二電路構 件中，該第二基板爲有機質絕緣基板較佳，藉此，富有可 撓性之有機質絕緣基板與玻璃基板的連接變容易。 此外，在該第一電路構件中，該第一基板爲半導體晶 片’該第二電路構件中，該第二基板爲玻璃基板，而且該 第二電路電極爲金屬電極電路較佳，藉此，將半導體晶片 直接實裝於玻璃基板上變容易。 冬 .，V% 1352109 本發明更提供一種被覆粒子之製造方法，其爲導電粒 子表面的至少一部份被絕緣性材料被覆的被覆粒子之製造 方法，其特微係包括將該導電粒子分散於含有高分子電解 質之溶液中，使該高分子電解質吸附在該導電粒子表面的 至少一部份上後進行洗淨之第1階段，與將吸附有該高分 子電解質之該導電粒子，分散於含有無機氧化物微粒子之 分散液中，使該無機氧化物微粒吸附在該導電粒子及該高 分子電解質表面的至少一部份上後進行洗淨之第2階段， 交互重複進行之吸附步驟。 依據該相關的被覆粒子之製造方法，可有效率的製造 上述本發明的各向異導電性黏著劑組成物中所使用的被覆 粒子。 〔發明之效果〕 依據本發明，可提供即使連接間距變爲窄間距時，亦 可充分的抑制因爲分散的導電粒子凝聚而於相鄰電路電極 間發生短路，可得到優異的長期連接信賴性之各向異導電 性黏著劑組成物、使用其之各向異導電性薄膜、電路構件 之連接構造、及被覆粒子之製造方法。 〔實施發明之最佳形態〕 以下’依情況參圖面詳細說明關於本發明較適合的實 施形態’再者’圖面中，同一要素使用同一符號，省略重 複的說明。 -10 - 1352109 本發明的各向異導電性黏著劑組成物，其係用於使第 一基板的主面上形成第一電路電極之第一電路構件、與第 二基板的主面上形成第二電路電極之第二電路構件，在該 第一電路電極與該第二電路電極爲對向配置狀態下連接之 各向異導電性黏著劑組成物，其特徵係含有黏著劑、及導 電粒子表面的至少一部份被含有高分子電解質與無機氧化 物微粒子的絕緣性材料被覆之被覆粒子。 作爲構成本發明的各向異導電性黏著劑組成物之黏著 劑，例如使用熱反應性樹脂與硬化劑的混合物，所使用的 黏著劑較佳可列舉環氧樹脂與潛在性硬化劑的之混合物。 潛在性硬化劑，可列舉咪唑系、醯肼系、三氟化硼-胺錯 合物、鏑鹽、胺醯亞胺、聚胺的鹽、雙氰胺等，另外，黏 著劑可使用自由基反應性樹脂與有機過氧化物的混合物、 或藉由紫外線等之能量線的照射而硬化的光硬化性樹脂。 上述環氧樹脂，可單獨使用或混合使用2種以上之由 環氧氯丙烷與雙酚A或F、AD等所衍生的雙酚型環氧樹 脂、由環氧氯丙烷與苯酚酚醛清漆或甲酚酚醛清漆衍生的 環氧酚醛清漆樹脂、具有含萘環骨架之萘系環氧樹脂、環 氧丙基胺、環氧丙基醚、聯苯、脂環式等之1分子內具有 2個以上的環氧丙基之各種環氧化合物等。此等環氧樹脂 ，使用雜質離子（Na+、C1 _等） '或水解性氯等減少至 3 OOppm以下的高純度品，這一點由防止電致遷移的觀點 而言較佳。 各向異導電性黏著劑組成物中’爲了降低黏著後的應 -11 - 1352109 力，或爲了提高黏著性，可混合丁二烯橡膠、丙烯酸橡膠 、苯乙烯-丁二烯-苯乙烯橡膠、腈·丁二烯橡膠、聚矽氧烷 橡膠等。此外，各向異導電性黏著劑組成物可使用糊狀或 薄膜狀者，爲了使各向異導電性黏著劑組成物成爲薄膜狀 ’其有效作法係摻合苯氧樹脂、聚酯樹脂、聚醯胺樹脂等 之熱塑性樹脂作爲薄膜形成性高分子，此等的薄膜形成性 高分子對於反應性樹脂的硬化時的應力緩和具有效果，特 別是薄膜形成性高分子具有羥基等官能基時，因爲提高黏 著性而較佳。薄膜形成係藉由使至少由環氧樹脂、丙烯酸 橡膠、潛在性硬化劑所成的黏著劑組成物溶解或分散於有 機溶劑而液狀化，將其塗佈於剝離性基材上，於硬化的活 性溫度以下去除溶劑而進行。此時所使用的溶劑，因爲芳 香族烴系與含氧系的混合溶劑使材料的溶解性提高而較佳 0 本發明之構成各向異導電性黏著劑組成物之被覆粒子 ，係導電粒子的表面的至少一部份被含有高分子電解質及 無機氧化物微粒子之絶緣性材料被覆而成者。在此，圖1 係以模擬方式表示本發明中之被覆粒子的其中一例的外觀 圖’如圖1所示，被覆粒子1係導電粒子6的表面的至少 一部份具有被含有高分子電解質7及無機氧化物微粒子8 之絶緣性材料9被覆之構造。再者，本發明中，導電粒子 6表面的至少一部份經被覆的狀態之意，係指用顯微鏡確 認時，如圖1所示，大粒徑的粒子上撒滿小粒徑的粒子之 狀態。 -12 - 1352109 本發明中，構成被覆粒子1的導電粒子6，例如含有 Au、Ag、Ni、Cu或焊劑等金屬之粒子，由聚苯乙稀等的 高分子所成的球狀的核材的表面上形成Au、Ag、Ni、Cu 、焊劑等的導電層所成的粒子較佳。此外，導電粒子6係 在具有導電性的粒子的表面上，形成Su、Au、焊劑等表 面層者亦可。 導電粒子6的粒徑，係必須小於使用各向異導電性黏 著劑組成物連接之電路構件的電極的最小的間隔，而且， 電極的高度有偏差時，大於高度的偏差較佳。導電粒子6 的平均粒徑以1〜l〇//m爲佳，2〜更佳，平均粒徑低 於lym，則會有粒子的分級變難的傾向，若超過l〇#m ，則會有於窄間距的電極間易發生短路的傾向。 本發明中之被覆粒子1，係上述導電粒子6的表面被 含有高分子電解質7及無機氧化物微粒子8之絕緣性材料 9所成的絕緣性皮膜被覆，此處，絕緣性材料9，係高分 子電解質7與無機氧化物微粒子8交互層合所成者。 被覆粒子1的具體製造方法，較佳爲使用包含（1) 將該導電粒子6分散於含有高分子電解質7之溶液中，使 該高分子電解質7吸附在該導電粒子6表面的至少一部份 上後進行洗淨（rinse)之第1階段、與（2)將吸附該高 分子電解質7之該導電粒子6，分散於含有無機氧化物微 粒子8之分散液中，使該無機氧化物微粒子8吸附在導電 粒子6及高分子電解質7表面的至少一部份上後進行洗淨 (rinse)之第2階段，交互重複進行之吸附步驟之方法。 -13- 1352109 於上述吸附步驟中，第1及第2階段可至少各進行1 次，亦可交互進行2次以上，第1及第2階段重複2次以 上時’對於第1次的第1及第2階段後之吸附了高分子電 解質7及無機氧化物微粒子8之導電粒子6，再度藉由第 1及第2階段使高分子電解質7及無機氧化物微粒子8被 吸附，藉由含有交互重複此第1及第2階段之吸附步驟， 可有效率的製造被導電粒子6的表面以高分子電解質7與 無機氧化物微粒子8交互層合的絕緣性材料9被覆之被覆 粒子1。在此，圖2係表示本發明中之被覆粒子1之製造 方法的其中之一實施形態之步驟圖。如圖2(a)〜（c)所 示’藉由第1階段’使導電粒子6的表面的至少一部份上 吸附高分子電解質7’藉由第2階段，使導電粒子6及高 分子電解質7的表面的至少一部份上吸附無機物微粒子8 ，可得到被覆粒子1。 這樣的方法’稱爲交互層合法（Layer-by-Layer assembly)，交互層合法係由G. Decher者等在1992年發 表之形成有機薄膜的方法（Thin Solid Films，210/211, p83 1 ( 1 992 ))，此方法係在具有正電荷的聚合物電解質 (聚陽離子）與具有負電荷的聚合物電解質（聚陰離子） 的水溶液中，交互浸漬基材，藉由靜電吸引力吸附於基板 之聚陽離子與聚陰離子的組合，經層合後得到複合膜（交 互層合膜）。 交互層合法，因爲是藉由靜電引力，拉近形成於基材 上的材料的電荷、與溶液中之具有相反電荷的材料而進行 -14- 1352109 膜成長，故吸附進行而引起電荷的中和後，就不會再引起 超過此程度以上的吸附，所以，只要到達某飽和點爲止， 膜厚不會再往上增加》Lvov等發表將交互層合法應用在 微粒子，使用二氧化矽或二氧化鈦、二氧化鈽的各微粒子 分散液，使具有與微粒子的表面電荷相反電荷之高分子電 解質，藉由交互層合法進行層合之方法（La ngmuir、Vol. 13、（ 1997)p6195-62 03 )。使用此方法，則具有負的表 面電荷之二氧化矽微粒子、與具有其相反電荷的聚陽離子 之聚二烯丙基二甲基銨氯化物（PDDA )或聚乙烯亞胺（ PEI)等藉由交互層合，可形成二氧化矽微粒子與高分子 電解質被交互層合的微粒子層合薄膜。 導電粒子6浸漬於高分子電解質溶液或無機氧化物微 粒子的分散液後，在浸漬於具有相反電荷之微粒子分散液 或高分子電解質溶液前，藉由僅用溶劑洗淨以洗掉剩餘的 高分子電解質溶液或無機氧化物微粒子的分散液較佳，作 爲使用於如此洗淨之溶劑，有水、醇、酮等，一般，由去 除剩餘的高分子電解質溶液或無機氧化物微粒子的分散液 之觀點而言，使用比電阻値爲1 8M Ω · cm以上的離子交 換水（所謂超純水）。吸附在導電粒子6上之高分子電解 質7及無機氧化物微粒子8，因爲互相或以靜電方式吸附 在導電粒子6表面，故在此洗淨的步驟中不會造成剝離。 而且，因爲無機氧化物微粒子8表面的極性基（主要是羥 基）的分極，導電粒子6表面的例如金屬或部份的金屬氧 化物之靜電的相互作用（引力）亦作用，此外，爲了防止 -15- 1352109 相反電荷的溶液中摻入未吸附的高分子電解質7或無機氧 化物微粒子8’進行洗淨較佳。不進行此洗淨時，因爲擴 入而使溶液內混入陽離子、陰離子，會有引起高分子電解 質7與無機氧化物微粒子8的凝集或沈澱的情況。 高分子電解質7’可使用於水溶液中電離，而在主鏈 或側鏈上具有電荷的官能基之高分子（聚陰離子或聚陽離 子），此時，聚陰離子’一般而言，爲具有磺酸、硫酸、 羧酸等可攜帶負電荷之官能基者，例如可使用聚苯乙烯磺 酸（PSS )、聚乙烯硫酸（PVS )、葡聚糖硫酸、軟骨素 硫酸、聚丙烯酸（PAA )、聚甲基丙烯酸（PMA )、聚馬 來酸、聚富馬酸等。此外’聚陽離子，一般而言，爲具有 4級銨基、胺基等之可攜帶正電荷的官能基者，例如可使 用聚乙烯亞胺 （PEI )、聚丙烯胺鹽酸鹽（pah )、聚二 烯丙基二甲基銨氯化物（PDDA )、聚乙烯吡啶（PVP )、 聚三甲基甘胺酸、聚丙烯醢胺、及含有至少1種以上此等 之共聚物等。 此等的高分子電解質7中，爲了避免電致遷移或腐鈾 的發生，較佳爲不含有鹼金屬（Li、Na、K、Rb、Cs)離 子、鹼土類金屬（Ca、Sr、Ba、Ra)離子、及、鹵化物離 子（氟離子、氯化物離子、溴離子、碘離子）者。 此等的高分子電解質7，皆爲水溶性或可溶於水與有 機溶劑的混合液者，高分子電解質7的分子量，依所使用 的高分子電解質7的種類而不同，不能一槪而論，一般而 言，較佳爲3〇〇~2〇〇,〇〇〇程度；再者，溶液中的高分子電 -16- 1352109 解質7的濃度，一般而言，較佳爲〇_〇1〜10質量％;此外 ，高分子電解質溶液的pH，並沒有特別的限制。 本發明所使用的高分子電解質溶液，一般爲水或水與 水溶性的有機溶劑的混合溶劑中溶解高分子電解質7者， 可使用的水溶性的有機溶劑，可列舉例如甲醇、乙醇、丙 醇、丙酮、二甲基甲醯胺、乙腈等。 藉由使用此等高分子電解質7，可在導電粒子6的表 面上形成無缺陷且均勻的高分子電解質薄膜，即使電路電 極間隔爲窄間距亦可充分的確保絕緣性，應進行電連接的 對向電極間可得到連接電阻低且優異的電連接。 無機氧化物微粒子8，由含有由矽、鋁、鉻、鈦、鈮 、鋅、錫、鈽及鎂所成群所選出的至少一種元素之氧化物 所成者較佳，此等可單獨或混合二種以上使用，而且，此 等中由絕緣性優異而言，以控制粒子徑的水分散膠體二氧 化矽（Si 02 )最佳。如此的無機氧化物微粒子8的市售品 ，可列舉例如 SNOWTEX、SNOWTEX UP (以上、日產化 學工業公司製）、QUARTON PL系列（扶桑化學工業公司 製）等，由得到充分的絕緣信賴性之觀點而言，較希望分 散溶液中的鹼金屬離子及鹼土類金屬離子的合計的濃度爲 lOOppm以下，此外，較佳爲使用藉由金屬醇鹽的水解反 應之所謂的溶膠凝膠法所製造的無機氧化物微粒子。 無機氧化物微粒子8的大小，藉由BET法之比表面積 換算法或X線小角散射法所測量的平均粒徑，20nm至 500nm較佳。無機氧化物微粒子8的平均粒徑低於20nm 1352109 ，則會有吸附在導電粒子6的無機氧化物微粒子8無法充 分發揮作爲絕緣膜的機能，一部份變得容易發生短路的傾 向，另一方面，超過50〇nm，則會有連接時的加壓方向的 導電性不足的傾向。 此外，各向異導電性黏著劑組成物中之被覆粒子1的 含量，以各向異導電性黏著劑組成物中的固體成份的全部 體積作爲基準，以〇_1〜30體積％爲佳，〇.2~15體積％更佳 ，此含量低於〇. 1體積％，則會有導電性降低的傾向，超 過3 0體積％，則會有絕緣性降低的傾向。 本發明的各向異導電性黏著劑組成物，上述被覆粒子 1以外，可混入.分散無機質塡充材料，無機質塡充材料 ，並沒有特別的限制，可列舉例如熔融二氧化矽、結晶質 二氧化矽、矽酸鈣、氧化鋁、碳酸鈣等的粉末。無機質塡 充材料的摻合量，相對於黏著劑100質量份，以10〜200 質量份較佳。使各向異導電性黏著劑組成物的熱膨脹係數 降低’雖然無機質塡充材料的摻合量愈大愈有效果，但摻 合太多量’則會有因爲黏著性或連接部的黏著劑的排除性 降低而容易發生導通不良的傾向，摻合量太少，則無法使 熱膨脹係數充分的降低，故摻合量係相對於黏著劑丨〇 〇質 量份爲20〜90質量份更佳。此外，無機質塡充材料的平均 粒徑’由防止連接部的導通不良的觀點而言，以3#m以 下爲佳’此外’由防止連接時的樹脂的流動性的降低及晶 片的鈍化膜的受損的觀點而言，較希望使用球狀塡充劑。 無機質塡充材料’可與被覆粒子1 一起使用，此外，使用 -18- 1352109 各向異導電性黏著劑組成物形成各向異導電性薄膜，使黏 著劑層多層化時，可混入·分散於未使用被覆粒子1之層 〇 圖3係表示本發明的各向異導電性薄膜（電路連接用 黏著薄膜）的較適合之一實施形態之模式截面圖，圖3所 示的各向異導電性薄膜100，係將含有被覆粒子1與黏著 劑2之各向異導電性黏著劑組成物形成薄膜狀而成者。 各向異導電性薄膜1〇〇，例如可藉由將液狀的各向異 導電性黏著劑組成物以輥軋塗佈機塗佈在離型性薄膜上， 使其乾燥後，從離型性薄膜剝離而得到。離型性薄膜，較 適合使用經表面處理使其具有離型性之PET薄膜等。 此外，於各向異導電性薄膜1〇〇，可使黏著劑層多層 化，例如可爲使含有用於賦予各向異導電性之被覆粒子之 黏著劑層、與不含有被覆粒子或導電粒子之黏著劑層進行 層合後所成时二層構成的各向異導電性薄膜，或者含有被 覆粒子之黏著劑層的兩側上層合不含有被覆粒子或導電粒 子的黏著劑層之三層構成的各向異導電性薄膜。此等的多 層構成的各向異導電性薄膜，因爲於連接電極上可有效率 的捕獲導電粒子，故有利於窄間距連接。此外，考慮與電 路構件的黏著性，可對於各個對向的電路構件層合黏著性 優異的黏著薄膜後，進行電路構件彼此的連接。 圖4係表示依據本發明之電路構件之連接構造的較適 合之一實施形態之模式截面圖，圖4所示的電路構件之連 接構造200,係具有第一基板11及其主面上形成第一電路 -19- 1352109 電極12之第一電路構件1〇、與具有第二基板21及其主面 上形成第二電路電極22之第二電路構件20，藉由形成於 由上述本發明的各向異導電性黏著劑組成物或各向異導電 性薄膜1〇〇硬化的硬化物所成的第一及第二電路構件10、 20之間之電路連接構件100a進行連接者。於電路構件之 連接構造200，第一電路電極12與第二電極22爲對峙的 同時被進行電連接。 電路連接構件l〇〇a，係由上述本發明的各向異導電性 黏著劑組成物或各向異導電性薄膜1 00硬化的硬化物所成 者，含有上述的黏著劑2的硬化物2a及分散於其中的被 覆粒子1，而第一電路電極12與第二電路電極22透過被 覆粒子1進行電連接。 第一及第二電路構件10、20，只要是形成進行電連接 所必須的電極者即可，並沒有特別的限制，具體而言，可 列舉使用液晶顯示器所使用的ITO等形成電極之玻璃或塑 膠基板、印刷配線板、陶瓷配線板、可撓性配線板、半導 體矽晶片等，此等必要時可組合使用。如同上述，本實施 形態以印刷配線板或聚醯胺等有機物所成材質爲首，可使 用具有銅、鋁等金屬或ITO( indium tin oxide)、氮化砂 (SiNx )、二氧化矽（Si02)等無機材質之各種的表面狀 態之電路構件。 電路構件之連接構造200’例如藉由使第—電路構件 10、與上述的各向異導電性薄膜100、與第二電路構件20 ，於第一電路電極11與第二電路電極21對峙的狀態下依 -20- 1352109 上述順序層合後加熱及加壓，連接第一電路構件ίο與第 二電路構件20，使第一電路電極11與第二電路電極21進 行電連接之連接方法而得到。 於此方法中，首先，將形成於剝離性基材上的各向異 導電性薄膜100，在貼合於第二電路構件20上的狀態下加 熱及加壓而暫時黏著各向異導電性薄膜100，從使剝離性 基材（離型性薄膜）剝離起，將第一電路構件1〇 —邊配 合電路電極的位置一邊放置，可準備依序層合了第二電路 構件20、各向異導電性薄膜100及第一電路構件10之層 合體" 加熱及加壓上述層合體的條件，依各向異導電性薄膜 1 〇〇中的黏著劑2的硬化性而不同，可適當調整，以使各 向異導電性薄膜硬化後可得到充分的黏著強度。 【實施方式】 實施例 以下，藉由實施例更具體的說明本發明的內容，但本 發明並不拘限於此等實施例。 [實施例1] (被覆粒子的製作） 在樹脂粒子（平均粒徑的聚苯乙烯類球狀樹脂 粒子、Merk Chime公司製、商品名：ESTAPOR L300)的 表面上，藉由無電解鎳電鍍設置厚度9 0nm的鎳皮膜’更 -21 -
1352109 於其鎳皮膜上，藉由置換金電鍍而設置30nm的 得到作爲導電粒子之金屬膜被膜導電樹脂粒子。 接著，將所得到的導電粒子的表面，用以下 以絕緣性材料被覆。各使用陽離子性聚合物之聚 作爲高分子電解質，使用二氧化矽作爲無機氧化 ，首先，將聚乙烯亞胺水溶液（濃度30質量％、 公司製、商品名：EPOMIN P 1 000 )，用超純水！ cm )稀釋，調整爲濃度0.3質量％，此外，膠體 分散液（濃度20質量％、扶桑化學工業公司製、 QUARTON PL-13、平均粒徑130nm)亦用超純7J •cm)稀釋，調整爲濃度0.1質量％，再者，此 化矽分散液中的二氧化矽微粒子的表面電位（ 爲-2 0 m V。 藉由將上述導電粒子2g，加進上述聚乙烯亞 (濃度0.3質量％) 200g中後攪拌15分鐘，製 子的表面吸附聚乙烯亞胺之高分子電解質被覆粒 ，以孔徑1 // m的膜濾器（MILLIPORE公司製） 分子電解質被覆粒子，將其在膜濾器上用200g 洗淨2次，去除未被吸附的聚乙烯亞胺。接著， 膜濾器回收的高分子電解質被覆粒子，加到上述 化矽分散液（濃度〇· 1質量％ ) 200g中後攪拌1 製作高分子電解質被覆粒子的表面上吸附二氧化 之被覆粒子。然後，與上述同樣用孔徑l#m的 濾出被覆粒子，將其在膜濾器上用200g的超純 金皮膜， 的方法藉 乙烯亞胺 物微粒子 日本觸媒 :1 8M Ω · 二氧化矽 商品名： ；(18ΜΩ 膠體二氧 Γ電位） 胺水溶液 作導電粒 子。然後 過據出局 的超純水 藉由將從 膠體二氧 5分鐘， 矽微粒子 膜濾器過 水洗淨2 -22- 1352109 次，去除未被吸附的膠體二氧化矽微粒子，而且，爲了去 除水，用異丙醇200g洗淨被覆粒子，然後，將從膜濾器 回收的被覆粒子在8 0°C的烘箱內保管1小時，使異丙醇蒸 發，結果，得到在導電粒子的表面上，交互吸附作爲絕緣 粒子之聚乙烯亞胺與平均粒徑130ηιη的膠體二氧化矽所成 的被覆粒子。 (各向異導電性黏著劑組成物的製作） 依下述順序製作黏著劑溶液，首先，將苯氧樹脂（ Union Carbide公司製、商品名：PKHC) 100g、與丙稀酸 橡膠（丁基丙烯酸酯40質量份、乙基丙烯酸酯30質量份 、丙烯腈30質量份及環氧丙基甲基丙烯酸酯3質量份的 共聚物，重量平均分子量：85萬）75g，溶解於乙酸乙酯 400g中，得到固體成份30質量％的樹脂溶液。接著，將 含有微膠囊型潛在性硬化劑之液狀環氧樹脂（環氧當量 185、旭化成環氧股份有限公司製、商品名：N〇Vacure HX-3941 ) 300g，加到上述樹脂溶液中後攪拌，製作黏著 劑溶液。 接著，將上述被覆粒子分散於上述黏著劑溶液中，使 其相對於該黏著劑溶液中的固體成份100體積份成爲9體 積份，得到各向異導電性黏著劑組成物的溶液。 (各向異導電性薄膜的製作） 將所得到的溶液，用輥軋塗佈機塗佈於離型器（經聚 •〆 -23- 1352109 砂氧院處理的聚對苯二甲酸乙二醇酯薄膜、厚度40/ζπ1) 上’以90°C乾燥10分鐘後’形成厚度25//m的各向異導 電性黏著劑層，藉此，得到各向異導電性薄膜。 (電路構件之連接構造的製作） 依下述順序進行附有金凸塊（面積：30x90# m、間距 :10Vni、高度：15/zm'凸塊數：362)之晶片（1.7x 1.7mm、厚度：〇.5/zm)、與附有A1電路之玻璃基板（厚 度：〇_7mm)的連接。首先，將上述各向異導電性薄膜（2 xl 9mm) ’以 8 0 °C、0.9 8 ΜP a ( 1 〇 kg f/cm2 )的條件，藉由 加熱及加壓貼合於附有A1電路之玻璃基板後，從各向異 導電性薄膜剝離離型器，進行晶片的金凸塊與A1電路的 位置調整。 接著，以190°C、40g/凸塊、1〇秒間的條件，從晶片 上方進行加熱及加壓，進行真正連接，藉此，製作電路構 件之連接構造，於所得到的電路構件之連接構造，連接電 阻爲每1凸塊最高爲ΙΟΟιηΩ，平均爲30ιηΩ，相鄰的凸 塊間的絕緣電阻皆爲1χ1〇8Ω以上。此外，此等數値，被 確認以-40°C保持30分鐘後昇溫至100°C而以100°C保持 30分鐘之熱衝擊試驗進行1〇〇〇循環後，亦無變化，顯示 出優良的長期連接信賴性。 [比較例1] 除了使用未用絕緣性材料被覆表面之與實施例1相同 '·、4 -24- 1352109 的金屬膜被覆導電樹脂粒子作爲導電粒子’取代被覆粒子 以外，其餘與實施例1同樣作法，製作各向異導電性薄膜 〇 接著，使用所製作的各向異導電性薄膜’依下述順序 進行附有金凸塊（面積：40x90/zm、間距：10ym、高度 :15#m、凸塊數：362)之晶片（1.7x1.7mm、厚度：〇.5 β m )、與附有A1電路之玻璃基板（厚度：〇.7mm)的連 接。 首先，將上述各向異導電性薄膜（2x19mm)，以80 t、〇.9 8MPa ( 1 Okgf/cm2 )的條件，藉由加熱及加壓貼合 於附有A1電路之玻璃基板後，從各向異導電性薄膜剝離 離型器，進行晶片的金凸塊與A1電路的位置調整。 接著，以190°C、40g/凸塊、10秒間的條件，從晶片 上方進行加熱及加壓，進行真正連接，藉此，製作電路構 件之連接構造，所得到的電路構件之連接構造中，連接電 阻爲每1凸塊最高爲130ιηΩ，平均爲80ιηΩ，但相鄰的 凸塊間的絕緣性未被充分的確保，一部份的凸塊間隨著導 電粒子的凝聚而發生短路。 依據本發明的各向異導電性黏著劑組成物，因爲使用 導電粒子的表面均勻的被高分子電解質薄膜及無機氧化物 微粒子被覆的被覆粒子，故在相鄰電極間的間距爲1 5以m 以下的窄間距中即使被覆粒子凝聚，藉由含有高分子電解 質與無機氧化物微粒子之絕緣性皮膜，可抑制導電粒子間 的短路，可提高窄間距連接性，此外，薄膜狀的黏著劑在 -25- 1352109 操作性方面亦優異。 所以，本發明的各向異導電性黏著劑組成物，可適合 使用於爲了僅在連接時的加壓方向進行電連接（1) LCD 、電漿面板或有機EL面板與TAB或FPC、（2) TAB與 FPC、（3) LCD、電漿面板或有機EL面板與1C晶片、（ 4 ) 1C晶片與印刷基板等，連接信賴性亦優異。 〔產業上的可利用性〕 如上述說明，依據本發明，可提供即使連接間距變爲 窄間距時，亦可充分的抑制因爲分散的被覆粒子凝聚而於 相鄰電路電極間發生短路，可得到優異的長期連接信賴性 之各向異導電性黏著劑組成物、使用其之各向異導電性薄 膜、電路構件之連接構造、及被覆粒子之製造方法。 【圖式簡單說明】 [圖1]以模擬方式表示本發明中之被覆粒子的其中一 例的外觀圖。 [圖2]表示本發明中之被覆粒子之製造方法的其中之 一實施形態之步驟圖。 [圖3]表示本發明的各向異導電性薄膜的較適合之一 實施形態之模式截面圖。 [圖4]表示依據本發明之電路構件之連接構造的較適 合之一實施形態之模式截面圖。 -26- 1352109 【主要元件符號說明】 1 :被覆粒子 2 :黏著劑 6 :導電粒子 7:高分子電解質 8 :無機氧化物微粒子 9 :絶緣性材料 1 〇 :第一電路構件 1 1 :第一基板 12 :第一電路電極 20 :第二電路構件 21 :第二基板 22 :第二電路電極 100 :各向異導電性薄膜 100a :電路連接構件 2〇〇 :電路構件之連接構造 -27-

Claims (1)

1352109 年^助日修正;^ 第〇96Π5750號專利申請案中文申請專利範圍修正本 民國100年4月U日修正 十、申請專利範圍 1.—種各向異導電性黏著劑組成物，其係用於使第 一基板的主面上形成第一電路電極之第一電路構件、與第 二基板的主面上形成第二電路電極之第二電路構件，在該 第一電路電極與該第二電路電極爲對向配置狀態下連接之 Φ 各向異導電性黏著劑組成物， 其特徵係含有黏者劑、及導電粒子表面的至少一部份 被含有在水溶液中會電離且在主鏈或側鏈上爲具有電荷之 官能基之高分子電解質與無機氧化物微粒子的絕緣性材料 ' 被覆之被覆粒子。 2. 一種各向異導電性黏著劑組成物，其係用於使第 一基板的主面上形成第一電路電極之第一電路構件、與第 二基板的主面上形成第二電路電極之第二電路構件，在該 φ 第一電路電極與該第二電路電極爲對向配置狀態下連接之 各向異導電性黏著劑組成物， 其特徵係含有黏著劑、及導電粒子表面的至少一部份 被含有高分子電解質與無機氧化物微粒子的絕緣性材料被 覆之被覆粒子； 前述高分子電解質係聚陰離子或聚陽離子。 3.如申請專利範圍第1或2項之各向異導電性黏著 劑組成物，其中該被覆粒子係該高分子電解質與該無機氧 化物微粒子交互地靜電吸附於該導電粒子表面的至少一部 1352109 份上而成。 4. 如申請專利範圍第i或2項之各向異導電性黏著 劑組成物，其中該無機氧化物微粒子係由含有選自矽 '鋁 、鉻、鈦、鈮、鋅、錫、铈及鎂所成群的至少一種元素的 氧化物所成。 5. 如申請專利範圍第1或2項之各向異導電性黏著 劑組成物，其中該無機氧化物微粒子的平均粒徑爲 20~500nm的範圍內。 6. 如申請專利範圍第1或2項之各向異導電性黏著 劑組成物’該高分子電解質係不含鹼金屬離子、鹼土類金 屬離子及鹵化物離子者。 7. —種各向異導電性薄膜，其特徵係將如申請專利 範圍第1 ~6項中任一項之各向異導電性黏著劑組成物形成 薄膜狀而成。 8. —種電路構件之連接構造，其特徵係第一基板的 主面上形成第一電路電極之第一電路構件、與第二基板的 主面上形成第二電路電極之第二電路構件，藉由被設置在 該第一及第二電路構件之間之由申請專利範圍第1〜7項中 任一項之各向異導電性黏著劑組成物的硬化物所成的電路 連接構件’使該第一電路電極與該第二電路電極對峙並且 進行電連接。 9. 如申請專利範圍第8項之電路構件之連接構造， 其於該第一電路構件中，該第一基板爲玻璃基板，而且該 第一電路電極爲金屬電極電路，該第二電路構件中，該第 -2- 1352109 二基板爲有機質絕緣基板。 10. 如申請專利範圍第8項之電路構件之連接構造， 其於該第一電路構件中，該第一基板爲半導體晶片，該第 二電路構件中，該第二基板爲玻璃基板，而且該第二電路 電極爲金屬電極電路。 11. 一種被覆粒子之製造方法，其爲導電粒子表面的 至少一部份被絕緣性材料被覆的被覆粒子之製造方法，其 特徵係包括吸附步驟，於該吸附步驟中，交互地重複進行 將該導電粒子分散於含有高分子電解質之溶液中，使該高 分子電解質吸附在該導電粒子表面的至少一部份上後進行 洗淨之第1階段、與將吸附有該高分子電解質之該導電粒 子，分散於含有無機氧化物微粒子之分散液中，使該無機 氧化物微粒吸附在該導電粒子及該高分子電解質表面的至 少一部份上後進行洗淨之第2階段。
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CN101517831A (zh) 2009-08-26
WO2008038565A1 (en) 2008-04-03
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