JP6501211B2 - 半導体パッケージ用熱硬化性樹脂組成物とこれを用いたプリプレグ - Google Patents
半導体パッケージ用熱硬化性樹脂組成物とこれを用いたプリプレグ Download PDFInfo
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- JP6501211B2 JP6501211B2 JP2017560669A JP2017560669A JP6501211B2 JP 6501211 B2 JP6501211 B2 JP 6501211B2 JP 2017560669 A JP2017560669 A JP 2017560669A JP 2017560669 A JP2017560669 A JP 2017560669A JP 6501211 B2 JP6501211 B2 JP 6501211B2
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- epoxy resin
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Classifications
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L33/00—Compositions of homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and only one being terminated by only one carboxyl radical, or of salts, anhydrides, esters, amides, imides or nitriles thereof; Compositions of derivatives of such polymers
- C08L33/24—Homopolymers or copolymers of amides or imides
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
- C08J5/24—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
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Description
本出願は、2016年1月13日付の韓国特許出願第10−2016−0004390号に基づく優先権の利益を主張し、当該韓国特許出願の文献に開示されたすべての内容は本明細書の一部として含まれる。
アクリル系ゴム5〜20重量部および充填剤160〜350重量部を含み、
前記アクリル系ゴムは、重量平均分子量30×104〜65×104、粘度1,000〜6,000mPa.s、ガラス転移温度10℃〜50℃の物性を有し、
前記充填剤は、(メタ)アクリレートシラン化合物が充填剤の表面に結合されており、平均粒径が0.2μm〜1μmの第1無機充填剤と、(メタ)アクリレートシラン化合物が充填剤の表面に結合されており、平均粒径が20nm〜50nmの第2無機充填剤とを含む1種以上の混合物である、半導体パッケージ用熱硬化性樹脂組成物を提供する。
エポキシ樹脂
前記エポキシ樹脂は、通常、プリプレグ用熱硬化性樹脂組成物に使用されるものが使用可能であり、その種類に限定はない。
[化学式1]
前記シアネート樹脂は、下記化学式3で表される化合物からなる群より選択された1種以上であってもよい。好ましい一例を挙げると、前記シアネート樹脂は、ノボラック型シアネート樹脂、ビスフェノールA型シアネート樹脂、ビスフェノールE型シアネート樹脂、テトラメチルビスフェノールF型シアネート樹脂のビスフェノール型シアネート樹脂、およびこれらの一部トリアジン化されたプレポリマーが挙げられ、これらは、単独あるいは2種以上を混合して使用することができる。
[化学式3]
本発明は、既存の硬化剤として用いていたフェノールノボラックをベンズオキサジン樹脂に変更して使用することによって、反応速度を制御することができる。つまり、従来主に使用されてきたフェノールノボラック硬化剤は、一般に、ヒドロキシ基が自体構造に含まれて、常温からエポキシ樹脂などと反応して初期反応速度が速い。反面、本発明で使用するベンズオキサジン樹脂は、硬化剤としての役割を示し、150℃以上の温度でヒドロキシ基が生じる特性があり、これにより、常温または初期には反応がゆっくり起こるが、一定温度以上で反応に参加して反応速度を調節することが可能である。
本発明で特徴とするアクリル系ゴムは、樹脂組成物に含まれて低い硬化収縮率特性を示すことができる。また、前記アクリル系ゴムは、膨張緩和作用の効果をより一層高めることができる。
本発明の他の実施例によれば、前記熱硬化性樹脂組成物を繊維基材に含浸させて製造されたプリプレグが提供される。
本発明のさらに他の実施例によれば、前記プリプレグ;および加熱および加圧によって前記プリプレグと一体化された金属箔;を含む金属箔積層板が提供される。
次の表1から4のような組成の成分を混合した後、高速撹拌機にて400rpmの速度で混合して、実施例1〜6および比較例1〜9の感光性樹脂組成物(樹脂ワニス)を製造した。
エポキシ樹脂:ナフタレン系エポキシ樹脂(HP4710、DIC社)
BMI樹脂:ビスマレイミド系樹脂(BMI−2300、DAIWA社)
シアネートエステル樹脂:ノボラック型シアネート樹脂(PT−30S、Lonza社)
ベンズオキサジン樹脂:フェノールフタレインベンズオキサジン樹脂(XU8282、Hunstman社)
BT樹脂:Nanozine600、Nanokor社
アクリル系ゴムA:SG−P3−PT197(Mw65×104、Tg:12℃)、Nagase Chemtex Coporation
アクリル系ゴムB:SG−P3−MW1(Mw30×104、Tg:12℃)、Nagase Chemtex Coporation
アクリル系ゴムC:SG−P3(Mw85×104、Tg:12℃)、Nagase Chemtex Coporation
Filler A:メタアクリルシラン処理されたスラリータイプのフィラー、平均粒径0.5μm(SC2050MTM、Admantechs社)
Filler B:メタアクリルシラン処理されたスラリータイプのフィラー、平均粒径50nm(YA050C−MJE、Admantechs社)
Filler C:メタアクリルシラン処理されたパウダータイプのフィラー、平均粒径1μm(SFP−130MCMA、Denka社)
Filler D:エポキシシラン処理されたスラリータイプのフィラー、平均粒径0.5μm(SC2050MTE、Admantechs社)
Filler E:メタアクリルシラン処理されたスラリータイプのフィラー、平均粒径100nm(MEK−AC−5140Z、Nissan Chemical社)
Filler F:フェニルシラン処理されたスラリータイプのフィラー、平均粒径0.5μm(SC2050MTI、Admantechs社)
Filler G:フェニルアミノシラン処理されたスラリータイプのフィラー、平均粒径0.5μm(SC2050MTO、Admantechs社)
実施例および比較例で製造した銅箔積層板に対して、次の方法で物性を測定した:
IPC−TM−650(2.3.17)により、プリプレグ状態でカーバープレスを用いてRFを測定した。
銅箔積層板の断面を観察用試験片に作製した。走査型電子顕微鏡によりボイド(void)の有無を調べて成形性を評価した。
銅箔積層板の銅箔層をエッチングして除去した後、DMAとTMAを用いてガラス転移温度を測定した。
銅箔積層板の銅箔層をエッチングして除去した後、DMAを用いて測定した。
銅箔積層板の銅箔層をエッチングして除去した後、TMAを用いて測定した。
銅箔積層板の銅箔層をエッチングして除去した後、TMAを用いて測定した。加熱(heating)→冷却(cooling)区間を経て、寸法(dimetnsion)変化の差を確認した。
デスミア評価で、全体的な工程条件の雰囲気はアルカリ性であり、工程はswelling、permanagement、netralizingの工程の順に進行させた。溶液は市販のAtotech社製溶液を使用した。
Claims (12)
- エポキシ樹脂、ビスマレイミド樹脂、シアネート樹脂、およびベンズオキサジン樹脂を含むバインダー100重量部を基準として、
アクリル系ゴム5〜20重量部および充填剤160〜350重量部を含み、
前記アクリル系ゴムは、重量平均分子量30×104〜65×104、粘度1,000〜6,000mPa.s、ガラス転移温度10℃〜50℃の物性を有し、
前記充填剤は、(メタ)アクリレートシラン化合物が表面に結合されており、
平均粒径が0.2μm〜1μmの第1無機充填剤と、(メタ)アクリレートシラン化合物が表面に結合されており、
平均粒径が20nm〜50nmの第2無機充填剤とを含む1種以上の混合物である、半導体パッケージ用熱硬化性樹脂組成物。 - 前記アクリル系ゴムは、
アクリル酸ブチル由来の繰り返し単位とアクリロニトリル由来の繰り返し単位とが含まれるアクリル酸エステル共重合体;
またはブタジエン由来の繰り返し単位が含まれるアクリル酸エステル共重合体である、請求項1に記載の半導体パッケージ用熱硬化性樹脂組成物。 - 前記アクリル系ゴムは、
炭素数2〜10の直鎖もしくは分枝鎖のアルキル基を有するアクリル酸アルキル由来の繰り返し単位をさらに含む、
請求項1または2に記載の半導体パッケージ用熱硬化性樹脂組成物。 - 前記充填剤は、
平均粒径が0.2μm〜1μmの第1無機充填剤と、
平均粒径20nm〜50nmの第2無機充填剤とを、
全体表面処理された充填剤の総重量を基準として、
10:90〜90:10の重量比で含む、
請求項1から3のいずれか1項に記載の半導体パッケージ用熱硬化性樹脂組成物。 - 前記バインダーは、
エポキシ樹脂20〜60重量%、
ビスマレイミド樹脂20〜70重量%、
シアネート樹脂30〜70重量%、
およびベンズオキサジン樹脂2〜10重量%を含む、
請求項1から4のいずれか1項に記載の半導体パッケージ用熱硬化性樹脂組成物。 - 前記ベンズオキサジン樹脂は、
ビスフェノールA型ベンズオキサジン樹脂、ビスフェノールF型ベンズオキサジン樹脂、フェノールフタレインベンズオキサジン樹脂、およびこれらのベンズオキサジン樹脂と硬化促進剤との混合物からなる群より選択された1種以上である、
請求項1から5のいずれか1項に記載の半導体パッケージ用熱硬化性樹脂組成物。 - 前記無機充填剤は、
シリカアルミニウムトリヒドロキシド、マグネシウムヒドロキシド、モリブデンオキシド、ジンクモリブデート、ジンクボレート、ジンクスタネート、アルミナ、クレー、カオリン、タルク、焼成カオリン、焼成タルク、マイカ、ガラス短繊維、ガラス微細パウダー、および中空ガラスからなる群より選択された1種以上である、
請求項1から6のいずれか1項に記載の半導体パッケージ用熱硬化性樹脂組成物。 - 前記エポキシ樹脂は、
ビスフェノールA型エポキシ樹脂、フェノールノボラックエポキシ樹脂、テトラフェニルエタンエポキシ樹脂、ナフタレン系エポキシ樹脂、ビフェニル系エポキシ樹脂、ジシクロペンタジエンエポキシ樹脂、およびジシクロペンタジエン系エポキシ樹脂とナフタレン系エポキシ樹脂との混合物からなる群より選択された1種以上である、
請求項1に記載の半導体パッケージ用熱硬化性樹脂組成物。 - 溶剤、硬化促進剤、難燃剤、潤滑剤、分散剤、可塑剤、およびシランカップリング剤からなる群より選択された1種以上の添加剤をさらに含む、
請求項1から10のいずれか1項に記載の半導体パッケージ用熱硬化性樹脂組成物。 - 請求項1から11のいずれか1項に記載の半導体パッケージ用熱硬化性樹脂組成物を繊維基材に含浸させて得られた
プリプレグ。
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