TWI342327B - - Google Patents

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Publication number
TWI342327B
TWI342327B TW095147924A TW95147924A TWI342327B TW I342327 B TWI342327 B TW I342327B TW 095147924 A TW095147924 A TW 095147924A TW 95147924 A TW95147924 A TW 95147924A TW I342327 B TWI342327 B TW I342327B
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TW
Taiwan
Prior art keywords
circuit
adhesive composition
electrode
connection
adhesive
Prior art date
Application number
TW095147924A
Other languages
English (en)
Other versions
TW200718769A (en
Inventor
Shigeki Katogi
Hoko Suto
Masami Yusa
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 TW200718769A publication Critical patent/TW200718769A/zh
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Publication of TWI342327B publication Critical patent/TWI342327B/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
    • C09J4/00—Adhesives based on organic non-macromolecular compounds having at least one polymerisable carbon-to-carbon unsaturated bond ; adhesives, based on monomers of macromolecular compounds of groups C09J183/00 - C09J183/16
    • 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
    • C09J4/00—Adhesives based on organic non-macromolecular compounds having at least one polymerisable carbon-to-carbon unsaturated bond ; adhesives, based on monomers of macromolecular compounds of groups C09J183/00 - C09J183/16
    • C09J4/06—Organic non-macromolecular compounds having at least one polymerisable carbon-to-carbon unsaturated bond in combination with a macromolecular compound other than an unsaturated polymer of groups C09J159/00 - C09J187/00
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F291/00—Macromolecular compounds obtained by polymerising monomers on to macromolecular compounds according to more than one of the groups C08F251/00 - C08F289/00
    • C—CHEMISTRY; METALLURGY
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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
    • 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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1342327 " (1) 九、發明說明 ^ 【發明所屬之技術領域】 本發明係有關’黏著劑組成物、電路連接用黏著劑組 * 成物、連接體及半導體裝置者。 【先前技術】 在半導體元件及液晶顯示元件中’使用以連接元件的 φ 種種構件爲冃的之各種黏著劑；此類黏著劑’必須具備以 黏著性爲苒，及耐熱性、高溫高濕狀態下之信賴性等多方 面的廣泛特性；又，黏著時使用之被黏物’係使用以印刷 配線板和聚醯亞胺等有機基材爲首，及銅、鋁等金屬和氧 化絪錫（ITO) 、SiN、Si〇2等具有各種各樣之表面狀態的 基材之故，各被黏物之混合分子設計’是屬必要者。 已往，使用以顯現高黏著性且具高信賴性之環氧樹脂 的熱硬化性樹脂，做爲半導體元件和液晶顯示元件用之黏 鲁著劑（例如特開平1 - 1 1 3 4 8 0號公號）；一般使用環氧樹脂 、與環氧樹脂具有反應性之酚樹脂等的硬化劑、促進環氣 樹脂與硬化劑反應之熱潛在性催化劑，做爲樹脂之構成成 份；熱潛在性催化劑爲決定硬化溫度及硬化速度之重要因 ' 素，由室溫（2 5 °C )下之貯存安定性及加熱時之硬化速度 . 的觀點而言，各種化合物均可使用，於實際步驟中’在 1 70〜250°C之溫度下硬化1〜3小時，可獲得所期望之黏著 :不過，隨著最近半導體元件之高集成化、液晶元件之高 精細化，元件間及配線間之間距也跟著狹窄化，加熱硬化 -5- 1342327 - (2) 時，恐會對週邊構件產生不良影響；而且由於 1 故，提高也產能力更有其必要性：低溫（1 00 . 短時間（1小時以內）’換句話說，耍求低溫 ’ 著；爲達成此低溫速硬化，必須使用低活性能 性能催化劑；如此之熱潛在性催化劑，很難兼 _ 近之貯存安定性。 最近’倂用（甲基）丙烯酸酯衍生物、與 φ 劑之過氣化物的游離基硬化型黏著劑，非常受 離基硬化，係由於反應活性種核之游離基，具 的反應性，可在短時間內硬化，而且，於游離 分解溫度以下，能安定的貯存；爲可使低溫速 溫附近之貯存安定性並存的硬化系（例如特開 2002-203427 號公號）。 【發明內容】 9 不過，游離基硬化系之黏著劑，於硬化時 甚大，與使用環氧樹脂之情況相比較，黏著強 其是對無機材質和金屬材質之基材的黏著強度 ，使用爲半導體元件和液晶顯示元件之黏著劑 - 得充分之性能（黏著強度等）。 - 本發明以提供一種爲游離基硬化系，同時 無機材質構成之基材顯現高黏著強度，於室溫 之貯存安定性優異，而且信賴性試驗後亦具有 黏著劑組成物、電路連接用黏著劑組成物、連 低成本化之 ^ 1 7 0 °C )、 速硬化之黏 量之熱潛在 備在室溫附 游離基引發 到注目：游 有非常旺盛 基引發劑之 硬化與在室 之硬化收縮 度較差，尤 降低；因而 時，不能獲 對以金屬及 (25。。）下 充分性能的 接體物及半 (S ) -6 - 1342327 ’ (3) 導體裝置爲目的。 ' 爲達成上述目的，本發明提供含有（a)〜（d)成分 之黏著劑組成物。 '' (a )熱塑性樹脂。 （b) 含有二個以上（甲基）丙烯醯基之游離基聚合 ^ 性化合物。 (c) 藉由150〜7 50 nm之光照射及/或80〜200°C之 φ 加熱，能產生游離基之硬化劑（以1 50〜75 0 nm之光照射 、或80〜20 0°C之加熱，或光照射與加熱併用，產生游離 基之硬化劑）。 (d )單獨於25 °C下之黏度爲1〇〜1〇〇〇 Pa · S的液狀 橡膠。 此黏著劑組成物中，對含有含（甲基）丙烯醯雄之游 離基聚含性化合物的游離基硬化系黏著劑組成物，添加以 授與薄膜形成性爲主要目的之熱塑性樹脂’更與上述具有 •特定黏度之液狀橡膠組合’可以達到對以金屬和無機材質 等構成之基材’具有高黏著強度的目的；還有，（甲基） 丙烯醯驻係指，丙烯醯基或（甲基）丙烯醯基之意（以下 均相同）。 此處，（d)液狀橡膠之主骨架’爲以選自聚異戊二 . 烯、聚丁二烯、苯乙烯一 丁二烯共聚物、丙烯腈- 丁二烯 共聚物、聚（羥基丙烯）、聚（羥基四甲稀）二醇、聚嫌 烴二醇及聚一 ε -己內酯所成群者，較爲適合；即是說’ (d)成份爲’以選自聚異戊二烯、聚丁二烯、苯乙烧一 1342327 • (4) 丁二嫌共聚物 '丙烧腈- 丁二烯共聚物、聚（羥基丙烯） '、聚（經基四甲稀）二醇、聚烯烴二醇及聚—ε -己內酯 及其改性物所成群者’單獨於2 5 0 r之黏度爲1 0〜1 0 0 0 P a ' .S的液狀橡膠較佳。 ，· 使用此等液狀橡膠，可以提高對黏著基材表面之濕潤 性、黏著強度。 u 黏著劑組成物爲’以含有對（a )成份1 〇 〇重量份、（ φ b)成份50〜250重量份、（c)成份〇5〜3〇重量份、及（ d )成份1〜5 0重量份’較爲適合；以此配合比率，可使黏 著強度、薄膜形成性、耐熱性、硬化速度、放置安定性等 更爲優異。 上述黏著劑組成物中’可以含有對黏著劑組成物總體 積之0 · 1〜3 0體積％的導電粒子；即是說，對黏著劑組成 物總計1〇〇體積部’可得含有0.1〜30體積％之導電粒子的 黏著劑組成物。 • 黏著劑組成物中配合導電粒子時，黏著劑組成物可以 做爲各向異性之導電性黏著劑使用；各向異性之導電性黏 著劑’例如以在電路基板之主面上，將有電路電極的電路 構件間相互連接，做爲電路連接用黏著劑組成物使用時， • 可以維持同一電路基板上之電路電極間的絕緣性，同時， - 可以經由導電粒子使對向之電路基板的電路電極間成電的 連接：即是說’本發明提供將由上述黏著劑組成物所成， 在電路基板之主面上具備電路電極的電路構件相互間，一 邊之電路構件的電路電極與另一邊之電路構件的電路電極 -8 - 1342327 • (5) ’以電的連接成對向而黏著之電路連接用黏著劑組成物。 ' 此電路連接用黏著劑組成物係，以使用上述之黏著劑 組成物’在具有對向電極之基板間，經由電路連接用黏著 ' 劑組成物’於對向基板間加壓，在加壓方向之電極間以電 -.的連接’使電路連接的方法，做爲電路連接用黏著劑組成 ^ 物’爲其特徵之電路連接用黏著劑組成物者。 本發明提供使用此電路連接用黏著劑組成物之下述連 φ 接體及半導體裝置。 連接體係，具備在第一電路基板之主面上具有第一電 路電極的第一電路構件、與在第二電路基板之主面上具有 第二電路電極的第二電路構件、和第-·及第二電路電極呈 對向狀態下，設置於第…及第二電路構件之問，第一及第 二電路電極間以電的連接，而成的電路連接構件者；上述 電路連接構件’爲由上述黏著劑組成物，或此硬化物所成 之連接體者。 • 半導體裝置係’具備具有連接電極之半導體元件、與 在電路基板之主面上具有電路電極之電路構件、和連接電 極及電路電極呈對向狀態下，設置於半導體元件及電路構 件間之連接電極及電路電極間以電連接的電路連接構件者 • :上述電路連接構件，爲由上述黏著劑組成物、或此硬化 - 物所成之半導體裝置者。 本發明提供’尤其是使用含有導電粒子之電路連接用 黏著劑組成物的下述連接體及半導體裝S。 連接體係，具備在第一電路基板之主面上具有第一電
： S -9- 1342327 . (6) 路電極的第一電路構件、與在第二電路基板之主面上具有 ' 第二電路電極的第二電路構件、和第一及第二電路電極呈 對向狀態下’設置於第一及第二電路構件間之第--及第二 •電路電極間以電連接的電路連接構件者：上述電路連接構 -- 件者：上述電路連接構件，爲由含有對黏著劑組成物全體 . 積之〇.〗〜30體積％的導電極子之黏著劑組成物、或此硬 化物所成；藉由該黏著劑組成物或此硬化物中之導電粒子 % ’使第一及第二電路電極間以電的連接，而成之連接體者 〇 半導體裝置係，具備具有連接電極之半導體元件、與 在電路基板之主面上具有電路電極之電路構件、和連接電 極及電路電極呈對向狀態下，設置於半導體元件及電路構 件之間’連接電極及電路電極間以電的連接，而成之電路 連接構件者；上述電路連接構件，爲山含有對黏著劑組成 物全體積之0. 1〜3 0體積％的導電粒子之黏著劑組成物、 0或此硬化物所成；藉由該黏著劑組成物或此硬化物中之導 電粒子，使連接電極及電路電極間以電的連接，而成之半 導體裝置。 〔用以實施發明之最佳形態〕 本發明中使用之（a )成份的熱塑性樹脂，可以使用 沒有特別限制之眾所周知者；此聚合物，可以使用聚醯亞 胺、聚醯胺、苯氧基樹脂類、聚（甲基）丙烯酸酯類、聚 醯亞胺類 '聚胺基甲酸酯類、聚酯類、聚乙烯醇縮丁醛類 -10- 1342327 ' (7) 等等；此等可單獨或兩種以上混合使用：而且， ' 屮，也可以含有矽氧烷鍵或氟取代基；此等爲混 相互間完全相溶者、或者發/-丨:.微相分離而呈白濁 ' 均適合使用；上述樹脂之分子量大者，容易獲得 -· 性；又，影響黏著劑之流動性的熔融黏度，可以 設定：分子量沒有特別的限制，一般重量平均 5,000 〜150,000較爲適合，以 10, 〇〇〇 〜80,000尤 鲁此値低於5,000時，薄膜形成性有劣化之傾向； 1 5 0,000時，與其他成份之相溶性有惡化之趨勢。 本發明中使用之（b )成份的含有二個以上 丙烯醯基之游離基聚合性化合物，沒有特別的限 使用眾所周知者。 具體的有，環氧（甲基）丙烯酸酯低聚物、 酯（甲基）丙烯酸酯低聚物、聚醚（甲基）丙烯 物、聚酯（甲基）丙烯酸酯低聚物等之低聚物、 #丙烷三（甲基）丙烯酸酯、聚乙二醇二（甲基） 、聚（烷）烯二醇（甲·基）丙烯酸酯、二環戊烯 )丙烯酸酯、二環戊烯氧基乙基（甲基）丙烯酸 二醇二（甲基）丙烯酸酯、二季戊四醇六（甲基 ' 酯、三聚異氰酸改性二官能（甲基）丙烯酸酯、 - 酸改性三官能（甲基）丙烯酸酯、2,2，—二（甲 醯氧基二乙基磷酸酯、2- （甲基）丙烯醯氧基 磷酸酯等之多官能（甲基）丙烯酸酯等等；此等 因應需求可以單獨或混合使用。 此等樹脂 合樹脂之 狀態者， 薄膜形成 廣範圍的 分子量以 其理想； 又，超過 (甲基） 制’可以 胺基甲酸 酸酯低聚 三羥甲基 丙烯酸酯 基（甲越 酯、季戊 )丙烯酸 三聚異氰 基）丙烯 乙基酸性 化合物， -11 - 1342327 • (8) (b )成份之添加量，對（a )成份1 〇 〇重量份，以5 Ο 〜250重量份較爲適合，以60〜50重量份更佳；添加量低 於5 Ο Μ量份時，硬化後之耐熱性恐會降低；又，超過2 5 〇 * 重量份時，於做爲薄膜使用之情況，其薄膜形成恐會下降 .ν 0 本發明中使用之（c)成份的藉由150〜750 nm之光照 射及/或8 0〜2 00 °C之加熱，而產生游離基的硬化劑，如 φ α -乙醯胺基苯酮衍生物和過氧化物、偶氮化合物等，沒 有特別的限制，可以使用眾所周知者；此等化合物，尤其 是由硬化溫度之設計容易的觀點而言，以過氧化物較爲適 合：能使用之過氧化物，可以簡便的參考顯示過氣化物之 分解越準的一分鐘半哀期溫度，一分鐘半哀期溫度，以40 °C以上200 °C以下較爲適合，其中以一分鐘半衰期溫度， 在60 °C以上1 70 °C以下最爲理想；一分鐘之半袞期溫度， 低於40 °C時，會损及保存安定性，超過200 °C時，硬化需 鲁要很長的時間。 如此之硬化劑有，二醯基過氧化物衍生物、過氧二碳 酸酯衍生物、過氧酯衍生物、過氧酮縮醇衍生物、二烷基 過氧化物衍生物、氫過氧化物衍生物等等。 • 二醯基過氧化物衍生物有，2,4 -二氯苯醯過氧化物 - 、3,5,5 -三甲基己醯過氧化物、辛醯過氧化物、十二醯 過氧化物、十八醯過氧化物、丁二醯過氧化物、苯醯過氧 甲苯、苯醯過氧化物等等。 過氧二碳酸酯衍生物有，二-正丙基過氧二碳酸酯、 -12- 1342327 • (9) 二異丙基過氧二碳酸酯、雙（4 -第三級丁基環己基）過 ' 氧二碳酸酯、二一 2 -乙氧基甲氣基過氣二碳酸酯、二（2 -乙基己基過氧）二碳酸酯、二甲氧基丁基過氧二碳酸酯 '、二（3 -甲基—3 -甲氧基丁基過氧）二碳酸酯等等。 . 過氧酯衍化物有’ 1，1 , 3，3 -四甲越丁茲過氧新癸酸酯 、1 -環己甚- 1-甲基乙基過氧十九酸酯、第三級己基過 氧新癸酸酯、第三級丁基過氧三甲基乙酸酯、1，1，3,3-四 φ 甲基丁基過氧-2-乙基己酸酯、2,5_二甲基_2,5—雙 (2-乙基己醯基過氧）己烷、2,5 —二甲基一 2,5—雙（2 一苯醯基過氧）己烷、1—環己基一 1—甲基乙基過氣一 2 -乙基己酸酯、第三級己基過氧- 2 -乙基己酸酯、第三 級丁基過氧異丁酸酯、1,1-雙（第三級丁越過氧）環己 烷、第三級己基過氣異丙基單碳酸酯、第三級丁基過氧-3,5,5 -三φ基己酸酯、第三級丁基過氧十二酸酯、2，5 -二甲基—2，5 -二（間—甲苯醯基過氧）己烷、第三級丁 φ驻過氧異丙基單碳酸酯、第三級丁基過氧- 2 -乙基己基 單碳酸酯、第三級己基過氧苯甲酸酯、第三級丁基過氧乙 酸酯等等。 過氧酮縮醇衍生物有，1，1 -雙（第三級己基過氣） * — 3,3，5-三甲基環己烷、I，丨—雙（第三級己基過氣）_ . 3,3,5_三甲基環己烷、1,1—雙（第三級丁基過氣）環十 二烷、2，2-雙（4,4 一二第三級丁基過氧環己越）丙烷、 2,2 -雙（第三級丁越過氧）癸烷等等。 二烷基過氧化物衍生物有，α，α ’ -雙（第三級丁基 -13- 1342327 * (10) 過氧）二異丙基苯、二異丙苯基過氧化物、2，5 一二甲基 - 2,5 -二（第一級丁基氧）己烷、第三級丁莛異丙苯基 過氣化物等等。 • 氫過氧化物類有，二異丙越苯氫過氣化物、異丙苯氫 • 過氧化物等等。 此等化合物’除單獨使用以外，亦可將兩種以上之化 合物混合使用。 • ( c )成份之添加量，對（a )成份1 〇 〇重量份，以〇. 5 〜3 0重量份較爲適合，以1〜2 0重萤份更佳；添加量低於 〇 · 5重堂份時，恐硬化不足；又，超過3 0重量份時，放置 安定性恐會下降。 本發明中使用之（d )成份的液狀橡膠，可以使用不 含溶劑等之液狀橡膠，眾獨於25 °C下之黏度爲1 0〜1 〇〇〇 Pa. S (以50〜800 Pa. S較適宜，以100〜500 Pa· S更佳 ，以150〜2 5 0 Pa · S最理想）的化合物；還有，此黏度係 0使用轉速控制式之旋轉黏度計（E型黏度計等），以錐與 板型之幾何運行，轉速爲〇.5〜50 rpm，於25 °C下測定之 値；此黏度低於1 〇 P a · S時，以黏著劑組成物做爲薄膜使 用之際，硬化後之彈性模數，恐有顯著下降之情形；超過 • 1 000 Pa · S時，造成薄膜之低流動化，恐會使黏著性降低 _ 〇 如此之液狀橡膠，以聚戊二烯、聚丁二烯、苯乙烯-丁二烯共聚物、丙烯腈-丁二烯共聚物、聚（羥基丙烯） 、聚（羥基四甲烯）二醇、聚烯烴二醇、聚—£ —己內酯 -14- (11) 1342327 及其改性物，特別適合：所謂改性物，係藉由含交 能性之單體的聚合等，將與主結構不同之結構導入 末端者之謂。 * 上述之具體例有，液狀聚異戊二烯、液狀聚丁 • 羧基末端液狀聚丁二烯、羥基末端液狀聚丁二烯 1,2 —聚丁二烯、羧基末端液狀1，2 —聚丁二烯、羥 液狀1 ,2 _聚丁二烯、液狀苯乙烯一 丁二烯橡膠、 φ 端液狀苯乙烯-T二烯橡膠、液狀丙烯腈- 丁二烯 聚合物末端含有羧基、羥基、（甲基）丙烯醯基、 基之液狀丙烯腈- 丁二烯橡膠、液狀羧基化之丁二 烯腈橡膠、羥基末端液狀聚（羥基丙烯）、烷氧基 基末端液狀聚（羥基丙烯）、液狀聚（羥基四甲烯 液狀聚（羥基丙烯）、液狀聚（羥基四甲烯）二醇 聚烯烴二醇、液狀聚-ε -己內酯等等。 其中以極性較高之液狀丙烯腈- 丁二烯橡膠、 φ末端含有羧基、羥基、（甲基）丙烯醯基、或嗎啉 狀丙烯腈-丁二烯橡膠、液狀羧基化丁二烯-丙烯 較爲適合，極性基之丙烯腈含有量以1 0〜6 0重量％ 使用如此極性高之液狀橡膠，可以提高黏著強度。 ： 此等化合物除單獨使用以外，也可以兩種以上 - 用。 (d )成份之添加量，對（a )成份1 00重量％ 50重量％，以10〜30重量％更爲適合；添加量低疗 %時，很難獲得高黏著強度：又，超過50重量％時 聯性官 支鏈和 二烯、 、液狀 基末端 羥基末 橡膠、 或嗎啉 烯-丙 甲矽烷 )二醇 、液狀 聚合物 基之液 腈橡膠 爲宜； 混合使 爲1〜 ^ 1重量 ，硬化 -15- - (12) 1342327 後黏著劑之物性，會顯著的下降，信賴性恐會降低 本發明所使用之導電粒子有，Au、Ag、Ni、 錫等之金屬粒子，和碳等等；又，也可以以非導電 * 璃、陶瓷、塑料等做爲核心，將上述之金屬、金屬 .. 碳等被覆於此核心；尤其是使用以上述金屬、金屬 碳等被覆於以塑料爲核心者、和熱熔融金酈粒子， 電粒子，由於具有加熱加壓之變型性，能吸收電極 φ 的離析不勻、連接時可增加與電極之接觸面積，而 接信賴性，極爲適宜；又，此等導電粒子之表面， 分子樹脂等被覆而成之微細粒子，可以抑制因導電 配合量增加時粒子相互之問的接觸而引起的短路， 電極電路間之絕緣性，此可單獨使用或與導電粒子 用。 此導電粒子之平均粒徑，由分散性、導電性之 言，以1〜1 8 m較爲適宜：平均粒徑低於1 μ m時 •電極相互間之電連接不完全，超過1 8 v m時，很難 電極間距離狹窄之高密度的電路構件。 導電粒子之使用量，沒有特別的限制；對黏著 物總體積，以含有0.1〜30體積％較適合，以0.1〜 1 %更理想；此値低於〇. 1體積％時，導電性有劣化 - ，超過3 0體積％時，將引起電路之短路；還有，體 依23 °C之硬化各成份的體積而決定，各成份之體積 用比重，由重量換算成體積；又，可以在量筒中置 成份不溶解不膨脹而可潤濕之適當溶媒（水、醇等
Cu、焊 性之玻 粒子、 粒子、 做爲導 之高度 提升連 更以高 粒子之 能提升 混合使 觀點而 ，電路 適用於 劑組成 10體積 之趨勢 積％係 ，可利 入對此 )，加 -16- 1342327 - (13) 入此成份，其所增加之體積’做爲其體積而求得。 ‘本發明之黏著劑組成物中，可以適當添加以烷氧基矽 烷衍生物、和矽氨烷衍生物爲代表之偶合劑及提升密著劑 ’ 、平坦劑等之黏著劑。 . 本發明之黏著劑組成物，爲提高交聯率之目的，除上 述（b )成份以外，可以適當添加，具有由於丙烯基、馬 來酸酐縮亞胺基、乙烯基等活性游離丛而聚合之官能基的 φ 化合物；具體的有，N -乙烯基咪唑、N -乙烯基吡啶、N -乙烯基吡咯烷酮、N -乙烯基甲醯胺、N —乙烯基己內 醯胺、4,4’ 一亞乙烯基-雙（N，N -二甲基苯胺）、N —乙 烯基乙醯胺、N，N -二甲基丙烯醯胺、N -異丙基丙烯醯 胺、N，N -二乙基丙烯醯胺、丙烯醯胺等等。 本發明之黏著劑組成物，爲提昇流動性之目的，可以 倂用單官能（甲基）丙烯酸酯；具體的有，季戊四醇（甲 基）丙烯酸酯、2 -氰基乙基（甲基）丙烯酸酯、環己丛 φ (甲基）丙烯酸酯、二環戊烯越（甲基）丙烯酸酯、二環 戊烯氧基乙基（甲基）丙烯酸酯、2— （2 -乙氧基乙氧基 )乙基（甲基）丙烯酸酯、2 -乙氧基乙基（甲基）丙烯 酸酯' 2 —乙基己基（甲基）丙烯酸酯、正己基（甲基） . 丙烯酸酯、2-羥基乙基（甲基）丙烯酸酯、羥基丙基（ - 甲基）丙烯酸酯、異冰片基（甲基）丙烯酸酯、異癸基（ 甲基）丙烯酸酯、異辛基（甲基）丙烯酸酯、正十二（院 )基（甲基）丙烯酸酯、2—甲氧基乙基（甲基）丙烯酸 酯、2 -苯氧基乙基（甲基）丙烯酸酯、四氫糠基（甲基 -17- 1342327 * (14) )丙烯酸酯、2 -(甲基）丙烯醯氣基乙碌 —二甲基胺基乙基（甲基）丙綠酸酯、N，N — 乙基（甲基）丙烯酸酯、N，N —二甲基胺基丙 丙烯酸酯、N，N —二甲基胺基丙基（甲基）丙 _· 甲基）丙烯醯基嗎啉等等。 本發明之黏著劑組成物，於常溫下爲糊狀 接使用其糊狀物；室溫下爲固體時，除加熱使 φ使用溶劑而糊狀化：可使用之溶劑，必須對黏 及黏著劑不具反應性，而且顯示充分之溶解性 特別的限制’以在常壓下之沸點爲5 0〜1 5 0 °C 點在50°C以下時，於室溫下放置，會有揮發之 用於開放系；又，沸點在1 5 0 °C以上時，溶劑 恐對硬化後之信賴性有不良影響。 本發明之黏著劑組成物，適合於形成薄膜 著劑組成物中’因應需求可加入溶劑等調成溶 鲁沸樹脂薄膜、聚對苯二甲酸乙二醇酯薄膜、脫 離性基材上，或在不織布等基材浸漬上述溶液 剝離性基材上’去除溶劑等，可做爲薄膜使用 形狀使用’由處理性等之觀點而言，更爲方便 • 本發明之黏著劑組成物，可用光照射及/ - 同時加壓而黏著；此等之倂用，可使於低溫及 著：光照射，以1 5 0〜7 5 0 nm之波長範圍的照 用低壓水銀燈、中壓水銀燈、高壓水銀燈、超 、氙氣燈、金屬鹵素燈等，以0.1〜10 J/cm2之 丨酸酯、N，N 二甲基胺基 基（甲基） 烯酸酯、（ 時，可以直 用外，可以 著劑組成物 ，對此沒有 者爲佳；沸 慮，不過使 難以揮發1 狀使用：黏 液，塗佈於 模紙等之剝 ，而附載於 ;以薄膜之 〇 或加熱，更 短時間內黏 射光爲宜* 高壓水銀燈 照射量硬化 S ) -18- (15) 1342327 較爲理想：加熱溫度沒有特別的限制，以50〜】7〇t爲宜 ，壓力’在不損害被黏物之範圍內，沒有特別的限制，一 般以0.1〜10 MPa較爲適合；此等之加熱及加壓，以在0.5 ' 秒〜3小時之範圍進行爲佳。 -· 本發明之黏著劑組成物，可以做爲，例如熱膨脹係數 _ 相異之不同種類被黏物的黏著劑使用；具體的說，可以做 爲各向異性導電黏著劑、銀糊狀物、銀薄膜等代表之電路 •連接材料、CSP用彈性體' CSP用塡不滿材料、LOC磁帶 等代表之半導體元件黏著材料使用。 本發明之電路連接用黏著劑組成物，爲由上述黏著劑 組成物所成，例如’如後述所述，可使用於電路構件相亙 之間的連接，而得連接體及半導體裝置。 參考所附圖樣’並說明連接體及半導體裝置之實施型 態如下；還有，在圖式說明中，於同一要索之同一符號， 不做重覆說明：又，圖式中之尺寸與實際之尺寸並不相同 •。 圖1爲，使用不含導電粒子之電路連接用黏著劑組成 物，與實施型態相關之連接體的示意剖面圖。 如圖1所示，連接體100具備有，在第-.·電路基板31之 • 主面31a上具有第一電路電極32的第一電路構件30、與在 - 第二電路基板4丨之主面41a上具有第二電路電極42的第二 電路構件4 0、和第一電路電極3 2與第二電路電極4 2呈對向 狀態下’設置於第一電路構件3 0與第二電路構件40之間’ 使第一電路電極32與第二電路電極42以電的連接而成之電 -19- (16) 1342327 路連接構件l〇c ;還有，電路連接構件i〇c爲，由電路連接 用黏著劑組成物1 〇 (上述黏著劑組成物可適用爲此電路連 接用黏著劑組成物）之硬化物所成；又，第一電路電極3 2 ’ 與第二電路電極4 2，爲以相互接在一起，而成電的連接。 • · 圖1所示之連接體1 〇〇，可用例如下述之方法製造而得 〇 首先’如圖2所示’準備第一電路構件3〇、第二電路 鲁構件4〇、及成型爲薄膜狀之電路連接用黏著劑組成物1 〇 ; 其次，將電路連接用黏著劑組成物1 0裝載於第二電路構件 4 0之形成第二電路電極4 2的面上：更於電路連接用黏著劑 組成物10之上，裝載使第-·電路電極32與第二電路電極42 成對向配置之第一電路構件3 0 ;接著，將介於第·電路構 件3 0與第二電路構件4 0之問的電路連接用黏著劑組成物1 〇 ’邊加熱邊硬化，同時在主面3 1 a、4 1 a之垂直方向加壓， 形成第一及第二電路構件3 0、40之間的電路連接構件1 〇c •，即得圖1之連接體1〇〇。 圖3爲，使用含有導電粒子之電路連接用黏著劑組成 物’與實施型態相關之連接體的示意剖面圖。 如圖3所示’連接體200具備有，在第一電路基板31之 ' 主面3 1 a上具有第一電路電極3 2的第一電路構件3 0、與在 - 第二電路基板41之主面41a上具有第二電路電極42的第二 電路構件40、和第一電路電極32與第二電路電極42呈對向 狀態下’設置於第一電路構件30與第二電路構件40之間， 使第一電路電極3 2與第二電路電極4 2以電的連接而成之電 -20- 1342327 ' (17) 路連接構件2 〇 c ;還有，電路連接構件2 0 c爲，導電粒子2 2 分散於樹脂組成物2 1中之電路連接用黏著劑組成物20的硬 化物（即是說’導電粒子2 2分散於樹脂組成物之硬化物 21c中者）者；在成對向配之第一電路電極32與第二電路 .， 電極4 2之問，藉由導電粒子2 2之連接兩電路電極，使兩電 路電極經由導電粒子22，而成電的連接。 圖3所示之連接體2 0 0，例如，如圖4所示，準備第一 鲁電路構件30、第二電路構件40、及形成薄膜狀之電路連接 用黏著劑組成物20，依上述圖1獲得連接體1 〇〇同樣的方法 可以製造而得；還有，電路連接用黏著劑組成物20爲，導 電粒子2 2分散於樹脂組成物2 1中者：上述黏著劑組成物（ 但是，爲不含導電粒子者），可以適用爲樹脂組成物2 1。 構成電路基板之材料有，半導體、玻璃、陶瓷等之無 機材料，聚醯亞胺、聚碳酸酯等之有機材料，玻璃纖維/ 環氧樹脂所成之複合材料等等；此等可以單獨或組合使用 •。
具有電路電極之電路構件的具體例有，液晶顯示元件 . 、磁帶承載組件（TCP )、雙層構成可撓性電路板（FPC )等等；此等組合，可做爲電路電極相互間成電的連接之 ' 連接體。 • 圖5爲，與實施形態相關之半導體裝置的透視圖；此 半導體裝置爲，在半導體元件之電極、與其對向之裝載用 基板（電路構件）的電極之間，以電路連接用黏著劑組成 物介入；於半導體元件之電極、與對向之裝載用基板（電 -21 - (18) 1342327 路構件）的電極加壓，加壓方向之電極間成電的連接，而 ' 連接電路之方法中，使用上述之黏著劑組成物做爲電路連 接用黏著劑組成物，所連接而成之半導體裝置的一例。 ’ 圖5所示之半導體裝置300具備有，半導體元件50、與 • 在電路基板6 1之主面6 1 a上具有電路逛極6 2的電路構件6 0 、和半導體元件50之連接電極及電路電極62呈對向狀態下 ，設置於半導體元件5 0與電路構件6 0之間的電路連接構件 φ 2 0c ;此處，電路電極62與半導體元件50之連接電極（如 圖6中之連接電極52所示）爲以電的連接而成者。 圆6爲，沿圖5之VI-VI線的剖面圖。 圖6所示之半導體裝置300具備有，在半導體元件本體 51之主面51a上爲有連接電極52之半導體元件50、與在電 路基板6 1之主面6 1 a上具有電路電極6 2之電路件6 0、和連 接電極52與電路電極62呈對向狀態下，設置於半導體元件 50與電路構件60之間，連接電極52與電路電極62以電的連 φ 接而成之電路連接構件20c;此處，電路連接構件20 c爲， 導電粒子22分散於樹脂組成物2 1中之電路連接用黏著劑組 成物20之硬化物（即是說，導電粒子22分散於樹脂組成物 之硬化物2 1 c中者），在成對向配置之連接電極52及電路 1 電極62之間，導電性粒子22連接兩電極，使兩電極相互之 • 間經由導電粒子22，而成電的連接。 半導體裝置3 00，準備半導體元件50、電路構件60及 電路連接用黏著劑組成物20，依上述圖1獲得連接體1 00同 樣的方法可以製造而得。 -22- (19) 1342327 半導體裝置之具體例爲，使做爲半導體元件之集成電 ' 路（1C )晶片、與晶片連接基板連接的裝置等。 【實施方式】 .· 〔實施例〕 以實施例具體的說明本發明如下；本發明對此沒有特 別的限制。 〔實施例1〜2、比較例1〕 將做爲（a )熱塑性樹脂之苯氣樹脂（優尼甕卡拜德 公司製，商品名爲PKHC，平均分子量45,〇〇〇 ) 40 g，溶解 於甲乙酮6 0 g中，調成固形份爲4 0重量％之溶液；使用做 爲（b)游離基聚合性化合物之三聚異Μ酸環氧乙烷改性 的二丙烯酸酯（柬亞合成股份有限公司製，商品名爲Μ -2 15)、及2 -(甲基）丙烯醯氧越乙基磷酸酯（共榮社股 • 份有限公司製，商品名爲來特酯Ρ-2Μ )，做爲（c )硬化 劑之1，1 _雙（第三級己基過氧）一 3,3,5 -三甲越環己烷 (曰本油脂股份有限公司製，商品名爲帕里去薩ΤΜΗ )， 做爲液狀橡膠之液狀丁腈橡膠（日本澤甕股份有限公司製 • ，商品名爲尼泊爾13121或尼泊爾DN 601 );此等液狀橡 • 膠，單獨於25°C下之粘度，使用東京計器股份有限公司製 之E型黏度EHD 2H7，以轉子之轉速1 rpm測定之，結果 尼泊爾1312爲183 Pa· S、尼泊爾DN 601爲262 Pa· S;又 ，以聚苯乙烯爲核心之粒子表面設置爲0.2 a m之鎳層；此 -23- (20) 1342327 鎳層之外側，設置厚度爲0.0 2 /i m之金屬；製作成平均粒 徑爲5 // m、比重爲2 · 5之導電粒子。 以如表1所示之固形份m量比調配，更將1.5體積％之 導電粒子分散配合’使用塗布裝置塗佈於厚度8 0 " m之氟 樹脂薄膜上’經70°C 1 〇分鐘之熱風乾燥，即得黏著劑層 之厚度爲1 5 // m的薄膜狀黏著劑。 表1 配合劑 實施例1 實施例2 比較例1 比較例2 熱塑性樹脂 PKHC 50 50 50 50 游離基聚合 M-215 45 45 45 45 性化合物 來特酯P-2M 5 5 5 5 硬化劑 帕里去薩TMH 3 3 3 3 液狀橡膠 尼泊爾1312 5 _ _· 尼泊爾DN601 _ 5 _ 固體橡膠 甩泊爾HF01 —— — _ 5
〔黏著強度、連接電阻之測定〕 使用由上述製法而得之薄膜狀黏著劑，將在厚度爲38 之聚酿亞胺薄膜上具有線寬50/im、問距lOOjwm、厚 度8 " m之銅電路5 00條的雙層可撓性電路板（FPC )、與 形成0.2 // m之氧化銦錫（ITO )薄層的玻璃（厚度爲1.1 nm、表面電阻爲20 Ω /□)，以熱壓黏合裝置（東麗工程 股份有限公司製，加熱方式爲固定加熱型），在1 6 0 t：、3 -24- (21) (21)1342327 PMa下施行1 0秒鐘之加熱加壓，爲寬2 mm之連接，即製得 連接體；此連接體之鄰接電路間的電阻値，以多點測定器 測定黏著剛完成、與在85 °C，85%相對濕度之高溫高濕槽 中經1 20小時後之電阻値，求出鄰接電路間之1 5〇處電阻的 平坦（X + 3 σ，σ爲標準誤差），即爲電阻値。 又，此連接體之黏著強度，依jlS— Ζ0237之標準，以 9 0度剝離法測定，並評估；此處，黏著強度之測定裝置係 採用東洋波魯多衛因股份有限公司製之田喜隆U T Μ · 4 (彔IJ 離速度爲50 mm/min、25°C );如上所述，進行連接體之 黏著強度 '連接電阻之測定，其結果如表2所示。 (表2 ) 連接電B &(Ω ) 黏著強违 ?(N/m) 黏著剛完成 1 2 0小時後 黏著剛完成 1 2 0小時後 實 施 例1 2.3 2.5 700 600 實 施 例2 1 .8 2.8 800 750 比 較 例1 2.8 8.4 200 150 比 較 例2 1 0 Ω以上 1 〇 Ω以上 230 200 〔比較例2〕 除實施例1中之液狀橡膠，以在2 5 °C下爲固體之丁腈 橡膠（日本澤甕股份有限公司製，商品名爲尼泊爾H F 0 1 )5重量份替代以外’其他都和實施例1同樣的製成薄膜狀 黏著劑：進行評估；還有，尼泊爾HF01在25 °C下爲固體 -25- ' (22) 1342327 之故，不能測定橡膠單獨之黏度。 實施例1〜2所得之黏著劑組成物，在黏著剛完成時及 在8 5 °C、8 5 %相對濕度之高溫高濕槽中經！ 2 〇小時後，均 顯現具有良好之連接電阻及黏著強度，並持有高耐久性； •針對此等’本發明中不使用液狀橡膠時（比較例1 )，雖 然黏著剛完成時顯示良好之數據，怛是在8 5 °C、8 5 %相對 濕度之高溫高濕槽中經1 2 0小時後，連接電阻上昇；而且 g黏著強度在黏著剛完成及在8 5 t、8 5 %相對濕度之高溫高 濕槽中經1 2 0小時後’均呈現極低之値；又，添加在2 5 t： 下爲固體狀之橡膠的比較例2中，連接電阻高而|L黏著強 度低，不能獲得滿意之連接體。 〔實施例3〕 將實施例1所得之薄膜狀黏著劑，施行真空包裝，於 4〇°C下放踣5天後，同樣施行與FPC及ITO之加熱壓著；黏 φ著剛完成時之連接電阻爲2 . 1 Ω、黏著強度爲7 6 0 N /m ; 在8 5 °C、8 5 %相對濕度之高溫高濕槽中經1 2 0小時後，連 接電阻爲2.9 Ω、黏著強度爲700 N/m;黏著剛完成時及 信賴性試驗後，均顯現與放置前相同之良好數據，具有優 異之保存安定性。 〔實施例4〕 除使用3重量份之1，1，3,3 —四甲基丁基過氧-2-乙基 己酸酯（曰本油脂股份有限公司製，商品名爲帕我庫達0 -26- (23) 1342327 )，做爲（c )硬化劑以外，其他都和實施例1同樣的製成 薄膜狀黏著劑，進行評估：其結果，黏著強度在黏著丨剛完 成時爲900 N/m，在8 5 °C、8 5 %相對濕度之高溫高濕槽中 ' 徑120小時後爲"750 N/m ;連接電阻在黏著剛完成時爲1 7 • Ω，在85°C、85%相對濕度之高溫高濕槽中徑uo小時後 爲2.3 Ω ;黏著剛完成及信賴性試驗後，均顯示良好之黏 著強度及連接電阻。 〔產業上利用性〕 使用本發明可以提供，顯示在低溫短時間硬化之高黏 著力，而且保存安定優越的黏著劑組成物、電路連接用黏 著劑組成物、連接體及半導體裝置。 【圖式簡單說明】 圖1爲，以不含導電粒子之電路連接用黏著劑組成物 φ連接，與實施形態相關之連接體的剖面圖。 圖2爲，第一電路構件與第二電路構件及薄膜狀電路 連接用黏著劑組成物（不含導電粒子）之示意剖面圖。 圖3爲，以含有導電粒子之電路連接用黏著劑組成物 ： 連接，與實施形態相關之連接體的示意剖面圖者。 - 圖4爲，第一電路構件、第二電路構件、及薄膜狀之 電路連接用黏著劑組成物（含有導電粒子）的模式示意剖 面圖。 圖5爲，與實施形態相關之半導體裝置的透視圖。 -27- (24) (24)1342327 圖6爲，沿著圖5之VI-V1線的剖面圖。 【主要元件符號說明】 1 〇 :電路連接用黏著劑組成物 l〇c :電路連接構件 20 :電路連接用黏著劑組成物 20c :電路連接構件 2 1 :樹脂組成物 2 1 c :樹脂組成物之硬化物 22 :導電粒子 3 0 :第一電路構件 3 1 :第一電路基板 31a:第一電路基板之主面 3 2 :第一電路電極 40 :第二電路構件 4 1 :第二電路基板 4 1 a :第二電路電極之主面 42 :第二電路電極 50 :半導體元件 5 1 :半導體元件本體 5 1 a :半導體元件本體之主面 52 :連接電極 60 :電路構件 61 :電路基板 -28- (25) (25)1342327
6 1 a :電路基板之主面 62 :電路電極 1〇〇 :連接體 2 0 0 :連接體 3 00 :半導體裝置 V I :(剖面線） (S ) -29 -

Claims (1)

1342327
十、申請專利範圍 第9 5 1 4 7 9 2 4號專利申請案 中文申請專利範圍修正本 民國99年7月23日修正 1 · 一種電路連接用黏著劑組成物，其係使在電路越 板之主面上具備電路電極的電路構件彼此間形成對向黏著 ’使其中之-電路構件的電路電極與另一電路構件的電路 電極’以電連接的蜇路連接用黏著劑組成物， 其特徵係含有：熱塑性樹脂、熱硬化性成分、平均粒 徑爲1〜1 8 e m之導電粒子及含有丙烯腊之共聚物所構成 的橡膠’對於該電路連接用黏著劑組成物全體積，含有該 導電粒子0 . 1〜3 〇體積％，前述該橡膠之丙烯腈含量爲！ 〇 〜6 0 % 〇 2·如屮請專利範圍第1項之電路連接用黏著劑組成 物’其中該橡膠爲液狀橡膠。 3·如申請專利範阚第1或2項之電路連接用黏著劑 組成物’其中該熱硬化性成分含有：具有二個以上之（甲 基）丙嫌醯基之游離基聚合性化合物及產生游離基的硬化 劑。
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KR100780135B1 (ko) 2007-11-28
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CN1288219C (zh) 2006-12-06
CN1692149A (zh) 2005-11-02
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US20090261483A1 (en) 2009-10-22
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US7576141B2 (en) 2009-08-18
CN1931947B (zh) 2013-05-22
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CN1931947A (zh) 2007-03-21
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