TWI288170B - Adhesive composition, adhesive composition for circuit connection, connected circuit structure, and semiconductor devices - Google Patents

Adhesive composition, adhesive composition for circuit connection, connected circuit structure, and semiconductor devices Download PDF

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Publication number
TWI288170B
TWI288170B TW092133727A TW92133727A TWI288170B TW I288170 B TWI288170 B TW I288170B TW 092133727 A TW092133727 A TW 092133727A TW 92133727 A TW92133727 A TW 92133727A TW I288170 B TWI288170 B TW I288170B
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Taiwan
Prior art keywords
circuit
electrode
adhesive composition
film
connection
Prior art date
Application number
TW092133727A
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English (en)
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TW200422372A (en
Inventor
Shigeki Katogi
Hoko Suto
Masami Yusa
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Hitachi Chemical Co Ltd
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Publication of TW200422372A publication Critical patent/TW200422372A/zh
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Publication of TWI288170B publication Critical patent/TWI288170B/zh

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    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J4/00Adhesives 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
    • C09J4/06Organic 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
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    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J4/00Adhesives 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
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    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08FMACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F291/00Macromolecular compounds obtained by polymerising monomers on to macromolecular compounds according to more than one of the groups C08F251/00 - C08F289/00
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    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J9/00Adhesives characterised by their physical nature or the effects produced, e.g. glue sticks
    • C09J9/02Electrically-conducting adhesives
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Description

1288170 πί 玖、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 種種構件爲目的之各種黏著劑;此類黏著劑,必須具備以 黏著性爲首,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 化銦錫(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 著劑(例如特開平1 一 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 氧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(25 °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 170〜25 0 °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- 1288170 * (2; 時,恐會對週邊構件產生不良影響;而且由於低成本化之 故,提高生產能力更有其必要性;低溫(100〜17CTC )、 短時間(1小時以內),換句話說,要求低溫速硬化之黏 著;爲達成此低溫速硬化,必須使用低活性能量之熱潛在 性能催化劑;如此之熱潛在性催化劑,很難兼備在室溫附 近之貯存安定性。 最近,倂用(甲基)丙烯酸酯衍生物、與游離基引發 劑之過氧化物的游離基硬化型黏著劑,非常受到注目;游 離基硬化,係由於反應活性種核之游離基,具有非常旺盛 的反應性,可在短時間內硬化,而且,於游離基引發劑之 分解溫度以下,能安定的貯存;爲可使低溫速硬化與在室 溫附近之貯存安定性並存的硬化系(例如特開20002 -203427號公號)。 【發明內容】 不過,游離基硬化系之黏著劑,於硬化時之硬化收縮 甚大,與使用環氧樹脂之情況相比較,黏著強度較差,尤 其是對無機材質和金屬材質之基材的黏著強度降低;因而 ,使用爲半導體元件和液晶顯示元件之黏著劑時,不能獲 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,同時對以金屬及 無機材質構成之基材顯現高黏著強度,於室溫(25 t )下 之貯存安定性優異,而且信賴性試驗後亦具有充分性能的 黏著劑組成物、電路連接用黏著劑組成物、連接體物及半 -6- (3)· 1288170 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150〜750 nm之光照射及/或80〜200°C之 加熱,能產生游離基之硬化劑(以150〜75 0 nm之光照射 、或80〜20 (TC之加熱,或光照射與加熱倂用,產生游離 基之硬化劑)。 (d) 單獨於25 °C下之黏度爲10〜1000 Pa· S的液狀 橡膠。 此黏著劑組成物中,對含有含(甲基)丙烯醯基之游 離基聚合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) 丙烯醯基係指,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、丙烯腈一 丁二稀 共聚物、聚(羥基丙烯)、聚(羥基四甲烯)二醇、聚烯 烴二醇及聚- 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、苯乙烯〜 -7- 1288170 (4)· 丁二烯共聚物、丙烯腈-丁二烯共聚物、 、聚(羥基四甲烯)二醇、聚烯烴二醇及 及其改性物所成群者,單獨於2 5 0 °C之黏月 • S的液狀橡膠較佳。 使用此等液狀橡膠,可以提高對黏著 性、黏著強度。 黏著劑組成物爲,以含有對(a )成f b)成份50〜250重量份、(c)成份0·5〜 d )成份1〜50重量份,較爲適合;以此配 著強度、薄膜形成性、耐熱性、硬化速度 更爲優異。 上述黏著劑組成物中,可以含有對黏 積之0.1〜30體積%的導電粒子;即是說 物總計1〇〇體積部,可得含有0.1〜30體積 黏著劑組成物。 黏著劑組成物中配合導電粒子時,黏 做爲各向異性之導電性黏著劑使用;各向 著劑,例如以在電路基板之主面上,將有 構件間相互連接,做爲電路連接用黏著劑 可以維持同一電路基板上之電路電極間的 可以經由導電粒子使對向之電路基板的電 連接;即是說,本發明提供將由上述黏著 在電路基板之主面上具備電路電極的電路 邊之電路構件的電路電極與另一邊之電路 聚(羥基丙烯) 聚一 ε —己內酯 I 爲 10 〜1 000 Pa 基材表面之濕潤 & 1 0 0重量份、( 3 0重量份、及( 合比率,可使黏 、放置安定性等 著劑組成物總體 ,對黏著劑組成 %之導電粒子的 著劑組成物可以 異性之導電性黏 電路電極的電路 組成物使用時, 絕緣性,同時, 路電極間成電的 劑組成物所成, 構件相互間,一 構件的電路電極 -8- 1288170 (5r ,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 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之間,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置。 連接體係,具備在第一電路基板之主面上具有第一電 -9 - 1288170 (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一及第二 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0 · 1〜3 0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,爲由含有對黏著劑組成 物全體積之0.1〜30體積%的導電粒子之黏著劑組成物、 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)丙燒酸酯類 '聚 醯亞胺類、聚胺基甲酸酯類、聚酯類、聚乙燒醇縮丁醒類 -10· 1288170 外 等等;此等可單獨或兩種以上混合使用;而且,此等樹脂 屮,也可以含有矽氧烷鍵或氟取代基;此等爲混合樹脂之 相互間完全相溶者、或者發生微相分離而呈白濁狀態者, 均適合使用;上述樹脂之分子量大者,容易獲得薄膜形成 性;又,影響黏著劑之流動性的熔融黏度,可以廣範圍的 設定;分子量沒有特別的限制,一般重量平均分子量以 5,000〜1 50,000較爲適合,以1 0,000〜80,000尤其理想; 此値低於5,000時,薄膜形成性有劣化之傾向;又,超過 1 5 0,0 00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(甲基) 丙烯醯基之游離基聚合性化合物,沒有特別的限制,可以 使用眾所周知者。 具體的有,環氧(甲基)丙烯酸酯低聚物、胺基甲酸 酯(甲基)丙烯酸酯低聚物、聚醚(甲基)丙烯酸酯低聚 物、聚酯(甲基)丙烯酸酯低聚物等之低聚物、三羥甲基 丙烷三(甲基)丙烯酸酯、聚乙二醇二(甲基)丙烯酸酯 、聚(烷)烯二醇(甲基)丙烯酸酯、二環戊烯基(甲基 )丙烯酸酯、二環戊烯氧基乙基(甲基)丙烯酸酯、季戊 二醇二(甲基)丙烯酸酯、二季戊四醇六(甲基)丙烯酸 酯、三聚異氰酸改性二官能(甲基)丙烯酸酯、三聚異氰 酸改性三官能(甲基)丙烯酸酯、2,2 / —二(甲基)丙 烯醯氧基二乙基磷酸酯、2-(甲基)丙烯醯氧基乙基酸 性磷酸酯等之多官能(甲基)丙烯酸酯等等;此等化合物 ,因應需求可以單獨或混合使用。 -11 - 1288170 • (8)_ (b)成份之添加量,對(a)成份100重量 〜25 0重量份較爲適合,以60〜50重量份更佳; 於5 0重量份時,硬化後之耐熱性恐會降低;又 重量份時,於做爲薄膜使用之情況,其薄膜形成 本發明中使用之(c)成份的藉由150〜750 射及/或80〜200 °C之加熱,而產生游離基的硬 α -乙醯胺基苯酮衍生物和過氧化物、偶氮化合 有特別的限制,可以使用眾所周知者;此等化合 是由硬化溫度之設計容易的觀點而言,以過氧化 合;能使用之過氧化物,可以簡便的參考顯示過 分解基準的一分鐘半衰期溫度,一分鐘半衰期溫 °C以上20 (TC以下較爲適合,其中以一分鐘半衰 在60 °C以上170 °C以下最爲理想;一分鐘之半衰 低於40 °C時,會損及保存安定性,超過200 °C時 要很長的時間。 如此之硬化劑有,二醯基過氧化物衍生物、 酸酯衍生物、過氧酯衍生物、過氧酮縮醇衍生物 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,2,4一二氯苯醯 、3,5,5—三甲基己醯過氧化物、辛醯過氧化 醯過氧化物、十八醯過氧化物、丁二醯過氧化物 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 份,以50 添加量低 ,超過250 恐會下降 n m之光照 化劑,如 物等,沒 物,尤其 物較爲適 氧化物之 度,以40 期溫度, 期溫度, ,硬化需 過氧二碳 、二烷基 過氧化物 物、十二 、苯醯過 碳酸酯、 -12- 0)* 1288170 二異丙基過氧二碳酸酯、雙(4 一第三級丁基環己基)過 氧二碳酸酯、二一 2 —乙氧基甲氧基過氧二碳酸酯、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 —甲基一 3—甲氧基丁基過氧)二碳酸酯等等。 過氧酯衍生物有,1,1,3,3-四甲基丁基過氧新癸 酸酯、1 -環己基一 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—四甲基丁基過氧一2 —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—苯醯基過氧)己烷、1—環己基—1 一甲 基乙基過氧一2 —乙基己酸酯、第三級己基過氧一 2-乙基 己酸酯、第三級丁基過氧異丁酸酯、1,1 一雙(第三級丁 基過氧)環己烷、第三級己基過氧異丙基單碳酸酯、第三 級丁基過氧一 3,5,5 —三甲基己酸酯、第三級丁基過氧 十二酸酯、2,5 —二甲基一 2,5 —二(間一甲苯醯基過氧 )己烷、第三級丁基過氧異丙基單碳酸酯、第三級丁基過 氧一 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,1,1一雙(第二級己基過氧) —3,3,5 —三甲基環己烷、1,1 一雙(第三級己基過氧 )一 3,3,5—三甲基環己烷、1,1 一雙(第三級丁基過 氧)環十二院、2,2-雙(4,4 —二第二級丁基過氧環己 基)丙烷、2,2-雙(第三級丁基過氧)癸烷等等。 二烷基過氧化物衍生物有,^^ / 一雙(第三級丁 -13- 1288170 (10) 基過氧)二異丙基苯、二異丙苯基過氧化物、2,5—二甲 基一 2,5-二(第三級丁基氧)己烷、第三級丁基異丙苯 基過氧化物等等。 氫過氧化物類有,二異丙基苯氫過氧化物、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0 · 5 〜3 0重量份較爲適合,以1〜20重量份更佳;添加量低於 〇 . 5重量份時,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,單獨於25 °C下之黏度爲〜1〇〇〇
Pa· S (以50〜800 Pa· S較適宜,以100〜500 Pa· S更佳 ,以1 5 0〜2 5 0 P a · S最理想)的化合物;還有,、此黏度係 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0 · 5〜5 0 r P m,於2 5 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、聚丁二燒、苯乙嫌一 丁二烯共聚物、丙烯腈- 丁二烯共聚物、聚(經基丙燒) 、聚(羥基四甲烯)二醇、聚烯烴二醇、聚一 6 一己內醋 -14- 1288170 (1^) 及其改性物,特別適合;所謂改性物,係藉由含交聯性官 能性之單體的聚合等,將與主結構不同之結構導入支鏈和 末ii而者之δ胃。 上述之具體例有,液狀聚異戊二烯、液狀聚丁二烯、 羧基末端液狀聚丁二烯、羥基末端液狀聚丁二烯、液狀1 ,2-聚丁二烯、羧基末端液狀1,2-聚丁二烯、羥基末 端液狀1,2-聚丁二烯、液狀苯乙烯一丁二烯橡膠、羥基 末端液狀苯乙烯-丁二烯橡膠、液狀丙烯腈-丁二烯橡膠 、聚合物末端含有羧基、羥基、(甲基)丙烯醯基、或嗎 啉基之液狀丙烯腈-丁二烯橡膠、液狀羧基化之丁二烯-丙烯腈橡膠、羥基末端液狀聚(羥基丙烯)、烷氧基甲矽 烷基末端液狀聚(羥基丙烯)、液狀聚(羥基四甲烯)二 醇液狀聚(羥基丙烯)、液狀聚(羥基四甲烯)二醇、液 狀聚烯烴二醇、液狀聚一 ε —己內酯等等。 其中以極性較高之液狀丙烯腈一 丁二烯橡膠、聚合物 末端含有羧基、羥基、(甲基)丙烯醯基、或嗎啉基之液 狀丙烯腈-丁二烯橡膠、液狀羧基化丁二烯-丙烯腈橡膠 較爲適合,極性基之丙烯腈含有量以10〜6 0重量%爲宜; 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,也可以兩種以上混合使 用。 (d)成份之添加量,對(a)成份1〇〇重量%,爲1〜 5〇重量%,以10〜30重量%更爲適合;添加量低於1重量 %時’很難獲得高黏著強度;又,超過50重量%時,硬化 -15- 1288170 (12) 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、Cu、焊 錫等之金屬粒子,和碳等等;又,也可以以非導電性之玻 璃、陶瓷、塑料等做爲核心,將上述之金屬、金屬粒子、 碳等被覆於此核心;尤其是使用以上述金屬、金屬粒子、 碳等被覆於以塑料爲核心者、和熱熔融金屬粒子,做爲導 電粒子,由於具有加熱加壓之變型性,能吸收電極之高度 的離析不勻、連接時可增加與電極之接觸面積,而提升連 接信賴性,極爲適宜;又,此等導電粒子之表面,更以高 分子樹脂等被覆而成之微細粒子,可以抑制因導電粒子之 配合量增加時粒子相互之間的接觸而引起的短路,能提升 電極電路間之絕緣性,此可單獨使用或與導電粒子混合使 用。 此導電粒子之平均粒徑,由分散性、導電性之觀點而 言,以1〜18//m較爲適宜;平均粒徑低於時,電路 電極相互間之電連接不完全,超過18#m時,很難適用於 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;對黏著劑組成 物總體積,以含有0.1〜30體積%較適合,以0.1〜10體積 %更理想;此値低於0.1體積%時,導電性有劣化之趨勢 ,超過3 0體積%時,將引起電路之短路;還有,體積%係 依23 °C之硬化各成份的體積而決定,各成份之體積,可利 用比重,由重量換算成體積;又,可以在量筒中置入對此 成份不溶解不膨脹而可潤濕之適當溶媒(水、醇等),加 -16- (13) 1288170 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、乙烯基等活性游離基而聚合之官能基的 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/ —亞乙烯基一雙(N,N —二甲基苯胺)、N 一乙烯基乙醯胺、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、環己基 (甲基)丙烯酸酯、二環戊烯基(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(烷 )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- 1288170 (14) )丙烯酸酯、2-(甲基)丙烯醯氧基乙基磷酸酯、N,N 一二甲基胺基乙基(甲基)丙烯酸酯、N,N—二甲基胺 基乙基(甲基)丙烯酸酯、N,N—二甲基胺基丙基(甲 基)丙烯酸酯、N,N—二甲基胺基丙基(甲基)丙烯酸 酯、(甲基)丙烯醯基嗎啉等等。 本發明之黏著劑組成物,於常溫下爲糊狀時,可以直 接使用其糊狀物;室溫下爲固體時,除加熱使用外,可以 使用溶劑而糊狀化;可使用之溶劑,必須對黏著劑組成物 及黏著劑不具反應性,而且顯示充分之溶解性,對此沒有 特別的限制,以在常壓下之沸點爲5 0〜1 5 0 °C者爲佳;沸 點在5 0 °C以下時,於室溫下放置,會有揮發之慮,不過使 用於開放系;又,沸點在1 5 0 °C以上時,溶劑難以揮發, 恐對硬化後之信賴性有不良影響。 本發明之黏著劑組成物,適合於形成薄膜狀使用;黏 著劑組成物中,因應需求可加入溶劑等調成溶液,塗佈於 沸樹脂薄膜、聚對苯二甲酸乙二醇酯薄膜、脫模紙等之剝 離性基材上,或在不織布等基材浸漬上述溶液,而附載於 剝離性基材上,去除溶劑等,可做爲薄膜使用;以薄膜之 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/或加熱,更 同時加壓而黏著;此等之倂用,可使於低溫及短時間內黏 著;光照射,以150〜750 nm之波長範圍的照射光爲宜, 用低壓水銀燈、中壓水銀燈、高壓水銀燈、超高壓水銀燈 、氙氣燈、金屬鹵素燈等,以0.1〜1 0 J / c m 2之照射量硬 -18- 1288170 (15) 化較爲理想;加熱溫度沒有特別的限制,以50〜170 °C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互 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,於同一要素之同一符號, 不做重覆說明;又,圖式中之尺寸與實際之尺寸並不相同 〇 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,在第一電路基板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32與第二電路電極42以電的連接而成之電 -19- 1288170 (16) 路連接構件l〇c ;還有,電路連接構件10c爲,由電路連接 用黏著劑組成物1 0 (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42,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30、第二電路 構件40、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 40之形成第二電路電極42的面上;更於電路連接用黏著劑 組成物10之上,裝載使第一電路電極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,將介於第一電路構 件3 0與第二電路構件40之間的電路連接用黏著劑組成物10 ,邊加熱邊硬化,同時在主面31a、41a之垂直方向加壓, 形成第一及第二電路構件30、40之間的電路連接構件10c ,即得圖1之連接體100。 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32與第二電路電極42以電的連接而成之電 -20- 1288170 (17) 路連接構件2 0 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22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42之間,藉由導電粒子22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200,例如,如圖4所示,準備第一 電路構件3 0、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2 0,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 〇 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 - 1288170 (18) 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61之主面61a上具有電路電極62的電路構件60 、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50與電路構件60之間的電路連接構件 20c ;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。 圖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上具有連接電極52之半導體元件50、與在電 路基板61之主面61a上具有電路電極62之電路件60、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 5 0與電路構件60之間,連接電極52與電路電極62以電的連 接而成之電路連接構件20c ;此處,電路連接構件20c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21c中者),在成對向配置之連接電極52及電路 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300,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 〇〇同 樣的方法可以製造而得。 -22- 1288170 (19) 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 )熱塑性樹脂之苯氧樹脂(優尼甕卡拜德 公司製,商品名爲PKHC,平均分子量45,000) 40 g,溶解 於甲乙酮60 g中,調成固形份爲40重量%之溶液;使用做 爲(b )游離基聚合性化合物之三聚異氰酸環氧乙烷改性 的二丙烯酸酯(東亞合成股份有限公司製,商品名爲Μ-215)、及2—(甲基)丙烯醯氧基乙基磷酸酯(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 一雙(第三級己基過氧)一3,3,5 —三甲基 環己烷(日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13 121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 25 5 7,以轉子之轉速1 rpm測定 之,結果尼泊爾13 12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 // m -23· 1288170 (20) 之鎳層;此鎳層之外側,設置厚度爲〇·〇2 // 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所示之固形份重量比調配,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80 // m之氟 樹脂薄膜上,經70 °C 10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 M-2 1 5 45 45 4 5 45 合性化合 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1 3 1 2 5 — — 一 尼泊爾DN601 一 5 一 — 固體橡膠 尼泊爾HF01 一 — 一 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3 8 // m之聚醯亞胺薄膜上具有線寬50 // m、間距100 // m、 厚度8#111之銅電路50()條的雙層可撓性電路板(??(:)、 -24- 1288170 (21) 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20Ω/Ε]),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 60 °C、3 PMa下施行10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120小時後之電阻値,求出鄰接電路間之150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JIS— Ζ023 7之標準,以 90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UTM — 4 ( 剝離速度爲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 ) 連接電阻(Ω ) 丨 黏著強度(N/m) 黏著剛完成 120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 0 Ω以上 230 200 〔比較例2〕 除實施例1中之液狀橡膠’以在25 °C下爲固體之丁腈 -25- 1288170 (22) 橡膠(日本澤甕股份有限公司製,商品名爲尼泊爾HF01 )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 t下爲固體 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85°C、85%相對濕度之高溫高濕槽中經120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,但是在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 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120小時後,均呈現極低之値;又,添加在25 °C 下爲固體狀之橡膠的比較例2中,連接電阻高而且黏著強 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 40°C下放置5天後,同樣施行與FPC及ITO之加熱壓著;黏 著剛完成時之連接電阻爲2.1 Ω、黏著強度爲760 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。 -26- 1288170 (23) 〔實施例4〕 除使用3重量份之1,1,3,3—四甲基丁基過氧一 2 — 乙基己酸酯(日本油脂股份有限公司製,商品名爲帕我庫 達〇 ),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 剛完成時爲9 0 0 N / m,在8 5 °C、8 5 %相對濕度之高溫高 濕槽中徑1 2 0小時後爲7 5 0 N / m ;連接電阻在黏著剛完成 時爲1 . 7 Ω,在8 5 °C、8 5 %相對濕度之高溫高濕槽中徑 120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 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 -27- 1288170 (24) 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。 圖6爲,沿著圖5之VI— VI線的剖面圖。 〔主要元件對照表〕 10 電 路 連 接 用 黏 著 劑 組 成 物 10c 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 1c 樹 脂 組 成 物 之 硬 化 物 22 導 電 企丄 子 30 第 — 電 路 構 件 3 1 第 一 電 路 基 板 3 1a 第 —* 電 路 基 板 之 主 面 32 第 一 電 路 電 極 40 第 二 電 路 構 件 41 第 二 電 路 基 板 4 1a 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 1a 半 導 體 元 件 本 體 之 主 面
•28- 1288170 (25) 52 連接電極 60 電路構件 6 1 電路基板 6 1a 電路基板之主面 62 電路電極 100 連接體 200 連接體 300 半導體裝置 VI (剖面線) -29-

Claims (1)

1288170 (1) 十、申請專利範圍 第92 1 3 3727號專利申請案 中文申請專利範圍修正本 民國96年6月8 日修正 1 · 一種薄膜狀黏著劑組成物,其特徵爲含有下述(a )〜(d )成份, (a )熱塑性樹脂, (b) 有二個以上(甲基)丙烯醯基的游離基聚合性 化合物, (c) 藉由150〜750 nm光照射及/或80〜200 °C之加 熱,而產生游離基的硬化劑, (d) 單獨於25 °C下黏度爲1〇〜1〇〇〇 Pa· S的液狀橡 膠。 2.如申請專利範圍第1項之薄膜狀黏著劑組成物,其 中(d)成份爲選自聚異戊二烯、聚丁二烯、苯乙烯一丁 二烯共聚物、丙烯腈一 丁二烯共聚物、聚(羥基丙烯)、 聚(羥基四甲烯)二醇、聚烯烴二醇、聚一 ε -己內酯及 其改質物所成群之,單獨於25 °C下黏度爲10〜1000 Pa· S 的液狀橡膠。 3 .如申請專利範圍第1或2項之薄膜狀黏著劑組成物 ,其中相對於(a )成份100重量份,(b )成份含有50〜 250重量份、(c)成份含有0.5〜30重量份、及(d)成份 含有1〜50重量份。 4.如申請專利範圍第1或2項之薄膜狀黏著劑組成物 1288170 (2). ,其中相對於黏著劑組成物總體積,則含有〇. 1〜 %之導電粒子。 5 · —種電路連接用薄膜狀黏著劑組成物,其 由申請專利範圍第1〜4項中任一項之薄膜狀黏著劑 所構成;在電路基板之主面上具備電路電極的電路 互間予以對向而黏著,使其一之電路構件的電路電 另一之電路構件的電路電極,以電的連接。 6. —種連接體,其特徵爲具備:在第一電路 主面上具有第一電路電極之第一電路構件;在第二 板主面上具有第二電路電極之第二電路構件;使上 及第二電路電極呈對向狀態下,設置於上述第一及 路構件之間,使上述第一及第二電路電極間以電的 電路連接構件,的連接體, 上述電路連接構件係由申請專利範圍第1〜4項 項之薄膜狀黏著劑組成物或其硬化物所成。 7. —種連接體,其特徵爲具備:在第一電路 主面上具有第一電路電極之第一電路構件;與在第 基板之主面上具有第二電路電極之第二電路構件; 述第一及第二電路電極呈對向狀態下,設置於上述 第二電路構件之間,使上述第一及第二電路電極間 接之電路連接構件,的連接體, 上述電路連接構件係由申請專利範圍第4項之 黏著劑組成物或其硬化物所成,藉由該薄膜狀黏著 物或其硬化物中導電粒子,以電的連接上述第一及 30體積 特徵係 組成物 構件相 極,與 基板之 電路基 述第一 第二電 連接之 中任一 基板之 二電路 在使上 第一及 以電連 薄膜狀 劑組成 第二電 -2- 1288170 (3) 路電極間。 8· —種半導體裝置,其特徵爲具備:具有連接電極 之半導體兀件;在電路基板之主面上具有電路電極的電路 構件;使上述連接電極及上述電路電極呈對向狀態下,設 置於上述半導體元件及上述電路構件之間,以電的連接上 述連接電極及上述電路電極間之電路連接構件,的半導體 裝置,上述電路連接構件係由申請專利範圍第1〜4項中任 一項之薄膜狀黏著劑組成物或其硬化物所構成。 9· 一種半導體裝置,其特徵爲具備:具有連接電極 之半導體元件;在電路基板之主面上具有電路電極的電路 構件;在使上述連接電極及上述電路電極呈對向狀態下, 設置於上述半導體元件及上述電路構件之間,以電的連接 上述連接電極及上述電路電極間之電路連接構件,的半導 體裝置,上述電路連接構件係由申請專利範圍第4項之薄 膜狀黏著劑組成物或其硬化物所成,藉由該薄膜狀黏著劑 組成物或其硬化物中導電粒子,以電的連接上述連接電極 及上述電路電極間。 -3-
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