TWI826536B - 樹脂組成物、附基材薄膜、金屬/樹脂層合物及半導體裝置 - Google Patents
樹脂組成物、附基材薄膜、金屬/樹脂層合物及半導體裝置 Download PDFInfo
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- TWI826536B TWI826536B TW108134325A TW108134325A TWI826536B TW I826536 B TWI826536 B TW I826536B TW 108134325 A TW108134325 A TW 108134325A TW 108134325 A TW108134325 A TW 108134325A TW I826536 B TWI826536 B TW I826536B
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- DOBFTMLCEYUAQC-UHFFFAOYSA-N naphthalene-2,3,6,7-tetracarboxylic acid Chemical compound OC(=O)C1=C(C(O)=O)C=C2C=C(C(O)=O)C(C(=O)O)=CC2=C1 DOBFTMLCEYUAQC-UHFFFAOYSA-N 0.000 description 1
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- 125000000951 phenoxy group Chemical group [H]C1=C([H])C([H])=C(O*)C([H])=C1[H] 0.000 description 1
- WVDDGKGOMKODPV-ZQBYOMGUSA-N phenyl(114C)methanol Chemical compound O[14CH2]C1=CC=CC=C1 WVDDGKGOMKODPV-ZQBYOMGUSA-N 0.000 description 1
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- 229910000679 solder Inorganic materials 0.000 description 1
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- 235000021122 unsaturated fatty acids Nutrition 0.000 description 1
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- 239000008096 xylene Substances 0.000 description 1
- 239000011787 zinc oxide Substances 0.000 description 1
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Abstract
本發明的課題為提供一種適合在鋁基基板之絕緣接著層的樹脂組成物。此樹脂組成物係其硬化物在0℃以下之低溫區域,為低彈性,且兼具耐熱性及接著性。
本發明的解決手段為一種樹脂組成物,其係包含(A)具有酸酐基之改質彈性體、(B)溶劑可溶性聚醯亞胺樹脂及(C)環氧樹脂。
Description
本揭示之一態樣係關於作為絕緣接著層使用之樹脂組成物。又,本揭示之一態樣係關於使用該樹脂組成物之附基材薄膜、金屬/樹脂層合物及半導體裝置。
在一般照明及汽車的照明,散熱設計變重要。為了散熱性能的提昇,使用鋁或銅之金屬基底基板被廣泛使用。金屬基底基板一般而言,係以於金屬構件(鋁或銅)之上重疊絕緣層(絕緣接著層),進而於其上重疊導體之銅箔的方式來構成。於此銅箔形成圖型。LED等之電子零件藉由焊接實裝。
絕緣層藉由添加熱傳導性的填料等,實現高熱傳導化。尤其是在將作為金屬構件之鋁作為基底之鋁基基板,因溫度變化導致之鋁伸縮的影響較大。因此,於實裝LED等之電子零件的焊接部分,有產生裂縫(焊接裂縫)的情況。作為減輕焊接裂縫之手法,認為低彈性化有絕緣層,將對金屬之伸縮的焊接之影響以絕緣層緩和之手法(參照專利文獻1)。一般而言,絕緣層變成越低溫變成越高彈
性。因此,在低溫絕緣層的彈性率為低,對焊接裂縫的抑制有效。尤其是在使用在汽車等之基板,有於寒冷地使用的情況。因此,即使在0℃以下之低溫區域,絕緣層為低彈性變重要。另一方面,基板所使用之絕緣層中,當然耐得住焊接實裝之耐熱性及對金屬構件之接著性亦重要。
[專利文獻1]日本特開2015-98504號公報
在本揭示之1個目的為提供一種適合於鋁基基板的絕緣接著層之如以下的樹脂組成物。此樹脂組成物係其硬化物在0℃以下之低溫區域,為低彈性,且兼具耐熱性及接著性。
為了達成上述之目的,關於本揭示之一態樣所提供之樹脂組成物(本樹脂組成物),其係包含:(A)具有酸酐基之改質彈性體、(B)溶劑可溶性聚醯亞胺樹脂及(C)環氧樹脂。
在本樹脂組成物,前述(A)較佳為被馬來酸酐改質之苯乙烯系彈性體。
在本樹脂組成物,前述(B)較佳為使四羧酸成分、與二聚物二胺進行反應所得之聚醯亞胺樹脂。
在本樹脂組成物,前述(A)的含量,較佳為相對於前述(A)、前述(B)及前述(C)之合計的固體成分質量,以質量%為40質量%以上。
本樹脂組成物較佳為進一步含有(D)無機填料。
又,於本樹脂組成物,前述(D)較佳為具有10W/m.K以上之熱傳導率的熱傳導性填料。
又,作為本揭示之其他態樣,係提供一種附基材薄膜,其係包含塑膠基材、與形成在前述塑膠基材的至少一面之包含本樹脂組成物之層。
又,作為本揭示之其他態樣,係提供一種金屬/樹脂層合物,其係包含金屬板或金屬箔、與形成在前述金屬板或金屬箔的至少一面之包含本樹脂組成物之層。
又,作為本揭示之其他態樣,係提供一種樹脂硬化物,其係本樹脂組成物之硬化物。
又,作為本揭示之其他態樣,係提供一種使用本樹脂組成物之半導體裝置。
本樹脂組成物係其硬化物在0℃以下之低溫
區域,為低彈性,且兼具耐熱性及接著性。因此,本樹脂組成物適合在鋁基基板之絕緣接著層。
以下,針對本揭示之一實施形態進行詳細說明。
在本揭示之一實施形態之樹脂組成物係包含(A)具有酸酐基之改質彈性體、(B)溶劑可溶性聚醯亞胺樹脂及(C)環氧樹脂。
針對在本揭示之一實施形態之樹脂組成物的各成分記載於以下。
(A)成分之具有酸酐基之改質彈性體,例如可藉由將酸酐及過氧化物與彈性體進行反應製造。作為具有酸酐基之改質彈性體,例如可列舉馬來酸酐改質之SEBS(聚苯乙烯/聚乙烯/聚丁烯/聚苯乙烯)共聚物、馬來酸酐改質之SBS(聚苯乙烯/聚丁二烯/聚苯乙烯)共聚物、馬來酸酐改質之SEPS(聚苯乙烯/聚乙烯/聚丙烯/聚苯乙烯)共聚物、馬來酸酐改質之SEP(聚苯乙烯/聚乙烯/聚丙烯)共聚物、馬來酸酐改質之SIS(聚苯乙烯/聚異戊二烯/聚苯乙烯)等之馬來酸酐改質苯乙烯系彈性體、馬來酸酐改質乙烯-丙烯共聚物、馬來酸酐改質乙烯-丁烯共聚物、馬來酸酐改質乙烯-丙烯酸甲酯共聚物、馬來酸酐改質乙烯-丙烯酸乙酯共聚
物及馬來酸酐改質乙烯-丙烯酸丁酯共聚物等。
(A)成分更佳為馬來酸酐改質苯乙烯系彈性體。馬來酸酐改質苯乙烯系彈性體樹脂特佳為馬來酸酐改質SEBS。
(A)成分之酸價較佳為0.1mgCH3ONa/g以上,更佳為1mgCH3ONa/g以上。酸價為0.1mgCH3ONa/g以上時,接著劑組成物的硬化充分,而得到良好之接著性及耐熱性。
被馬來酸酐改質之苯乙烯系彈性體的苯乙烯比率較佳為40%以下,更佳為30%以下,再更佳為28%以下,特佳為25%以下。苯乙烯比率過高時,在0℃以下之低溫區域的樹脂組成物之硬化物的彈性率提高,擔心焊接裂縫的發生。
(A)成分的含量相對於(A)成分、(B)成分及(C)成分之合計的固體成分質量以質量%,較佳為40%~95%,更佳為70~95%,再更佳為80%~95%。(A)成分較40%更少時,在0℃以下之低溫區域的樹脂組成物之硬化物的彈性率提高,擔心焊接裂縫的發生。(A)成分較95%更多時,由於相對地其他成分減少,故有焊接耐熱性惡化的可能性。
(B)成分之溶劑可溶性聚醯亞胺樹脂若可溶在溶劑即可,構造等並未特別限定。所謂可溶性,係意指於由以下
所選出之溶劑的至少一種,於23℃溶解20質量%以上。溶劑有烴系溶劑之甲苯及二甲苯、酮系溶劑之丙酮、甲基乙基酮、甲基異丁基酮、環己酮及環戊酮、醚系溶劑之1,4-二噁烷、四氫呋喃及二甘醇二甲醚、二醇醚系溶劑之甲基溶纖劑、乙基溶纖劑、丙二醇單甲基醚、丙二醇單乙基醚、丙二醇單丁基醚及二乙二醇甲基乙基醚、作為酯系溶劑之乙酸乙酯、乙酸丁酯、乳酸乙酯及γ-丁內酯、苄基醇、N-甲基吡咯烷酮、N,N-二甲基甲醯胺、以及N,N-二甲基乙醯胺。
(B)成分之溶劑可溶性聚醯亞胺樹脂可藉由使二胺與四羧酸成分於130℃以上的溫度進行反應,進行醯亞胺化反應而獲得。(B)成分之溶劑可溶性聚醯亞胺樹脂較佳為使四羧酸成分與二聚物二胺進行反應所得到之聚醯亞胺樹脂。此聚醯亞胺樹脂係接著性、柔軟性、強韌性及耐熱性優異。又,於(B)成分之溶劑可溶性聚醯亞胺,可將二聚物二胺之一部分被聚矽氧二胺取代。
作為於此使用之四羧酸成分,例如可列舉均苯四甲酸二酐、3,3’,4,4’-二苯甲酮四羧酸二酐、3,3’,4,4’-二苯碸四羧酸二酐、1,4,5,8-萘四羧酸二酐、2,3,6,7-萘四羧酸二酐、3,3’,4,4’-二苯醚四羧酸二酐、3,3’,4,4’-二甲基二苯基矽烷四羧酸二酐、3,3’,4,4’-四苯基矽烷四羧酸二酐、1,2,3,4-呋喃四羧酸二酐、4,4’-雙(3,4-二羧基苯氧基)二苯基硫化物二酐、4,4’-雙(3,4-二羧基苯氧基)二苯基碸二酐、4,4’-雙(3,4-二羧基苯氧基)二苯基丙烷二酐、
3,3’,4,4’-全氟異亞丙基二鄰苯二甲酸二酐、3,3’,4,4’-聯苯四羧酸二酐、雙(鄰苯二甲酸)苯基氧化膦二酐、p-伸苯基-雙(三苯基鄰苯二甲酸)二酐、m-伸苯基-雙(三苯基鄰苯二甲酸)二酐、雙(三苯基鄰苯二甲酸)-4,4’-二苯基醚二酐、雙(三苯基鄰苯二甲酸)-4,4’-二苯基甲烷二酐及4,4’-(4,4’-異亞丙基二苯氧基)二鄰苯二甲酸二酐等。
又,作為二聚物二胺,例如可列舉VERSAMINE551(商品名、BASF日本股份有限公司製;3,4-雙(1-胺基庚基)-6-己基-5-(1-辛烯基)環己烯)及VERSAMINE552(商品名、Cognis日本股份有限公司製;VERSAMINE551之氫化物)、以及PRIAMINE1075及PRIAMINE1074(皆為商品名、Croda日本股份有限公司製)等。
(B)成分之溶劑可溶性聚醯亞胺樹脂具有使四羧酸成分與二聚物二胺進行反應,以醯亞胺鍵聚合之構造。二聚物二胺之原料即二聚酸為二聚化碳數18之不飽和脂肪酸(油酸、亞麻油酸、亞麻酸等之混合物)者。進行二聚化時,藉由其反應機率,生成具有直鏈、脂環、雙鍵之脂環及具有芳香環者等。上述之二聚酸成為此等之混合物。將此直接胺化者為二聚物二胺。因此,聚合四羧酸成分與二聚物二胺所得之(B)成分之溶劑可溶性聚醯亞胺樹脂的分子構造,係混合物之二聚酸的各分子為不規則鍵結之構造,為複雜,特定有困難。作為可推測之分子構造,將如下述化學構造式所示者作為例列舉。分子構造被認為
是此等之混合物(此等構造式只是一個例。分子構造並非被限定於此等)。
上述之化學式中,n表示整數,R1、R2、R3及R4表示有機基。作為例,R1及R2表示-(CH2)n1-(CH=Cn2-(CH2)n3-CH3),有彼此相同的情況,亦有彼此不同的情況。R3及R4表示(CH2)n1-(CH=CH)n2-(CH2)n3-,有彼此相同的情況,亦有彼此不同的情況。n1及n3為0~18之整數,n2為0或1或2之整數。又,在二聚物二胺成分之碳數的合計為36。於(B)成分之溶劑可溶性聚醯亞胺樹脂,數平均分子量(Mn)較佳為10,000~20,000,更佳為12,000~18,000。數平均分子量可藉由GPC測定求出。
(B)成分的含量相對於(A)成分、(B)成分及(C)成分之合計的固體成分質量,以質量%較佳為1~45%,更佳為2~30%,再更佳為5~15%。(B)成分較45%更多時,在0℃以下之低溫區域之樹脂組成物之硬化物的彈性率變高,擔心焊接裂縫的發生等。另一方面,(B)成分較1%更少時,擔心接著性的降低及焊接耐熱性的降低。
作為(C)成分之環氧樹脂,例如可列舉雙酚A型環氧樹脂、雙酚F型環氧樹脂、酚酚醛清漆型環氧樹脂、脂環式環氧樹脂、矽氧烷型環氧樹脂、聯苯型環氧樹脂、縮水甘油基酯型環氧樹脂、縮水甘油基胺型環氧樹脂、乙內醯脲型環氧樹脂、具有萘骨架之環氧樹脂及具有蒽骨架之環氧樹脂。又,(C)成分之環氧樹脂如苯氧型之環氧樹脂般,可為分子量較大者。
關於本實施形態之樹脂組成物,於此所例示之化合物可單獨使用,亦可混合2個以上之化合物使用。(C)成分之環氧當量較佳為80~20,000g/eq,更佳為90~17,000g/eq,再更佳為90~500g/eq。
(C)成分的含量相對於(A)成分、(B)成分及(C)成分之合計的固體成分質量以質量%,較佳為1%以上,更佳為3~15%。(C)成分較1%更少時,擔心焊接耐熱性的降低。
本實施形態之樹脂組成物可進一步含有以下之成分作為任意成分。
(D)成分之無機填料較佳為選自二氧化矽、硫酸鋇、碳酸鈣、滑石、高嶺土、黏土、氮化硼、氮化矽、氮化鋁、碳化矽、氧化鎂、氫氧化鎂、碳酸鎂、氫氧化鋁及氧化鋁中之至少一種。
(D)成分之無機填料可因應本實施形態之樹
脂組成物的要求特性適當選擇。例如,重視降低樹脂組成物之硬化物的熱膨脹率(Coefficient of Thermal Expansion:CTE)時,(D)成分之無機填料較佳為二氧化矽。
另一方面,重視提高樹脂組成物之硬化物的熱傳導性時,作為(D)成分之無機填料,較佳為使用具有10W/m.K以上之熱傳導率者。
作為具有10W/m.K以上之熱傳導率的填料,可列舉氧化鋁(Alumina、Al2O3)、氧化鎂(MgO)、氧化鋅(ZnO)、氮化硼(BN)、碳化矽(SiC)、氮化鋁(AlN)、氮化矽(Si3N4)及鑽石等。從對於熱傳導率及濕度等之耐久性的觀點來看,具有10W/m.K以上之熱傳導率的填料,較佳為選自由氧化鋁及氮化硼所構成之群組中之至少1種。將各材料之熱傳導率測定結果之一例示於以下(單位為W/m.K)。Al2O3之熱傳導率為20~40。MgO之熱傳導率為45~60。ZnO之熱傳導率為54。BN之熱傳導率為30~80。SiC之熱傳導率為140~170。AlN之熱傳導率為150~250Si3N4之熱傳導率為30~80。鑽石之熱傳導率為1000~2000。
(D)成分之無機填料的形狀並未特別限定,可為球狀、不定形、鱗片狀等之任一種形態。作為(D)成分之無機填料,可使用凝聚體。
(D)成分之無機填料的平均粒徑較佳為0.1~100μm,更佳為0.1~50μm,再更佳為1~50μm。
在本說明書,平均粒徑係藉由雷射繞射.散射法所測定之於體積基準在粒度分布之積算值50%的粒徑。平均粒
徑例如可藉由雷射散射繞射法粒度分布測定裝置:LS13320(貝克曼庫爾特公司製、濕式)測定。
作為(D)成分之無機填料,使用具有10W/m.K以上之熱傳導率者的情況下,對樹脂組成物的添加量並未特別指定,可藉由必要之散熱性適當調節。例如,於硬化後為了得到2W/m.K以上之熱傳導率,對樹脂組成物之(D)成分之無機填料的添加量,相對於(A)成分、(B)成分及(C)成分之合計的固體成分100質量份,較佳為100~1200質量份,更佳為200~1000質量份。(D)成分之添加量過多時,在0℃以下之低溫區域之硬化物的彈性率提高。因此,擔心接著性降低等之發生。
又,具有10W/m.K以上之熱傳導率的填料的含量,在去除溶劑之本實施形態之樹脂組成物的全成分中,較佳為45體積%以上75體積%以下,更佳為50體積%以上70體積%以下。
作為(D)成分之無機填料,以降低CTE為目的,有使用二氧化矽的情況。此情況下,對樹脂組成物之(D)成分之無機填料的添加量,相對於(A)成分、(B)成分及(C)成分之合計的固體成分100質量份,較佳為10~700質量份,更佳為100~500質量份。
又,二氧化矽的含量在去除溶劑之本實施形態之樹脂組成物的全成分中,較佳為5體積%以上75體積%以下,更佳為30體積%以上70體積%以下。
(D)成分之無機填料的種類並未特別限制。
作為(D)成分之無機填料,可具有1種之填料,亦可併用2種以上之填料。使用2種以上之填料時,較佳為2種以上之填料的合計含量及平均粒子徑滿足上述之範圍。又,即使在使用平均粒徑不同之同種填料的情況下,合計含量及平均粒子徑亦以滿足上述之範圍較佳。
本實施形態之樹脂組成物可進一步含有矽烷耦合劑及咪唑系硬化觸媒等之硬化觸媒。
本實施形態之樹脂組成物的原料係包含上述(A)~(C)成分及如有必要添加之(D)成分、以及其他成分。可藉由將此等之原料溶解或分散等在有機溶劑,而得到本實施形態之樹脂組成物。用以溶解或分散等此等之原料的裝置並未特別限定。作為此裝置,可使用具備加熱裝置之攪拌機、溶解器、行星攪拌機、破碎機、三輥研磨機、球磨機及珠磨機等。又,可適當組合此等裝置使用。
本實施形態之樹脂組成物具有以下所示之合適的特性。
本實施形態之樹脂組成物的樹脂硬化物,在0℃以下之低溫區域,更具體而言,在-40℃~0℃之低溫區域,具有較低之彈性率。尤其是依後述之實施例所記載之順序所測定之本實施形態之樹脂組成物於-40℃之儲藏彈性率,為15GPa以下,較佳為10GPa以下,更佳為5GPa以下。若儲藏彈性率為上述之範圍,將本實施形態之樹脂組成物的硬化物使用在車載用電子零件等之用途時,有於實裝該電子零件之焊接部分,降低陷入裂縫之虞。
本實施形態之樹脂組成物例如可於150℃以上250℃以下,較佳為於180℃以上220℃以下的溫度熱硬化30~180分鐘。
作為(D)成分之無機填料,使用具有10W/m.K以上之熱傳導率者時,提高本實施形態之樹脂組成物的樹脂硬化物之熱傳導性。具體而言,以後述之實施例所記載之順序測定熱傳導率時,得到2W/m.K以上之熱傳導率。因此,作為鋁基基板等之金屬基底基板的絕緣接著層,使用實施形態之樹脂組成物時,散熱性良好。
本實施形態之樹脂組成物的樹脂硬化物具有充分之接著強度。具體而言,於本實施形態之樹脂組成物的樹脂硬化物,以後述之實施例所記載之順序所測定之70μm銅箔接著力為15N/10mm以上,較佳為20N/10mm以上。
本實施形態之樹脂組成物的樹脂硬化物具有高耐熱性。具體而言,在以後述之實施例所記載之順序實施之焊接耐熱性試驗,本實施形態之樹脂組成物的樹脂硬化物的耐熱性滿足280℃ 3min,較佳為滿足300℃ 3min。
本實施形態之附基材薄膜係具有聚酯樹脂、聚乙烯樹脂、聚對苯二甲酸乙二酯樹脂等之塑膠基材、與形成在此塑膠基材的至少一面之包含本實施形態之樹脂組成物之層。本實施形態之金屬/樹脂層合物係具有銅、鋁等之金屬板或金屬箔、與形成在此金屬板或金屬箔的至少一面之包含本實施形態之樹脂組成物之層。此等藉由於塑
膠基材或是金屬板或金屬箔的至少一面,塗佈本實施形態之樹脂組成物後並進行乾燥而獲得。
將樹脂組成物塗佈在塑膠基材或是金屬板或金屬箔之方法並未特別限定。惟,此塗佈方法從薄膜化.膜厚控制的點來看,較佳為微凹版法、槽模法及刮刀法。由槽模法,例如可形成包含具有5~500μm的厚度之樹脂組成物之層。
乾燥條件可因應使用在樹脂組成物之有機溶劑的種類及量、以及塗佈的厚度等適當設定。乾燥條件例如可於50~120℃定為1~30分鐘左右。
本實施形態之半導體裝置係為了半導體裝置之構成要素的層間接著,而使用本實施形態之樹脂組成物者。具體而言,例如於本實施形態之半導體裝置,為了電子零件與基板之層間接著等,使用有本實施形態之樹脂組成物。或於本實施形態之半導體裝置,於包含電子零件之裝置內使用本實施形態之樹脂組成物。
以下,由實施例更詳細說明本實施形態。惟,本實施形態並非被限定於此等之實施例。
以下述表所示之摻合,將指定量之各彈性體樹脂(A-1,A-2,A’)、各樹脂(B-1,B-2,C)及甲苯取放在容器,使用加
熱攪拌機進行加熱溶解,並冷卻至室溫。然後,於容器計量指定量之填料(D-1,D-2,D-3)及硬化觸媒(E),藉由自轉.公轉式之攪拌機(Mazerustar)(商品名)、倉敷紡績股份有限公司製)攪拌混合3分鐘。然後,在濕式微粒化裝置(MN2-2000AR吉田機械興業股份有限公司製)進行分散,使用甲苯調整黏度。藉此,調製包含樹脂組成物之溶液。
樹脂組成物之作成時所使用之成分係如以下。
(A-1)馬來酸酐改質苯乙烯系彈性體(SEBS)、M1913(商品名)、旭化成化學股份有限公司製、苯乙烯比率30%、酸價:10mgCH3ONa/g
(A-2)馬來酸酐改質苯乙烯系彈性體(SEBS)、M1943(商品名)、旭化成化學股份有限公司製、苯乙烯比率20%、酸價:10mgCH3ONa/g
(B-1):依下述順序合成之溶劑可溶性聚醯亞胺樹脂
於具備攪拌機、分水器、溫度計及氮氣導入管之反應容器,作成包含市售之芳香族四羧酸二酐(BTDT-UP(商品名)、Evonik日本股份有限公司製)210.0g、環己酮1008.0g及甲基環己烷201.6g之溶液。然後,將此溶液加熱至60℃。其次,將市售之二聚物二胺(PRIAMINE(商品名)
1075、Croda日本股份有限公司製)341.7g滴下在此溶液。然後,於140℃耗費10小時,進行此溶液之醯亞胺化反應。然後,進行溶劑之減壓餾除及甲苯取代。藉此,得到溶劑可溶性聚醯亞胺樹脂之溶液(不揮發分30.1%)。進行GPC測定時,數平均分子量(Mn)為15000。
(B-2):依下述順序合成之溶劑可溶性聚醯亞胺樹脂
於具備攪拌機、分水器、溫度計及氮氣導入管之反應容器,作成包含市售之芳香族四羧酸二酐(BTDT-UP(商品名)、Evonik日本股份有限公司製)190.0g、環己酮912.0g及甲基環己烷182.4g之溶液。然後,將此溶液加熱至60℃。其次,將市售之二聚物二胺(PRIAMINE(商品名)1075、Croda日本股份有限公司製)288.1g及市售之聚矽氧二胺(KF-8010(商品名)、信越化學工業製)24.7g滴下在此溶液。然後,於140℃耗費10小時,進行此溶液之醯亞胺化反應。藉此,得到聚醯亞胺樹脂溶液(不揮發分30.8%)。進行GPC測定時,數平均分子量(Mn)為14000。
(C)雙酚A型環氧樹脂、828EL(商品名)、三菱化學股份有限公司製
(A’)無馬來酸改質之苯乙烯系彈性體(SEBS)、G1657(商品名)、Kraton Polymer日本股份有限公司製、苯乙烯比率13%、酸價:0mgCH3ONa/g
作為具有10W/m.K以上之熱傳導率的熱傳導性填料,係使用(D-1)~(D-3)。
(D-1):球狀氧化鋁、DAW-0735(商品名)、Denka股份有限公司製、平均粒徑7μm
(D-2):鱗片狀氮化硼、Platelets0075(商品名)、3M日本股份有限公司製、平均粒徑7.5μm
(D-3):凝聚氮化硼、FP-40(商品名)、Denka股份有限公司製、平均粒徑40μm
(E):咪唑系硬化觸媒、2-苯基-4,5-二羥基甲基咪唑、2PHZ-PW(商品名)、四國化成工業股份有限公司製
對於依上述之順序製作之樹脂組成物,實施以下之評估。
將包含依上述之順序所得之樹脂組成物的溶液塗佈在塑膠基材(實施脫模處理之PET薄膜)的單面,於100℃乾燥5分鐘。藉此,製作厚度約100μm之薄片。藉由將製作之薄片在200℃、5MPa的條件,沖壓60分鐘使其硬化,而得到樹脂硬化物。將此樹脂硬化物切出40mm×10mm之帶狀。使用SII奈米科技公司製之DMS6100,求出在帶狀之
樹脂硬化物於-40℃之儲藏彈性率。
將所得之結果用下述基準評估。
儲藏彈性率(-40℃)
A 5GPa以下
B 超過5GPa且為10GPa以下
C 超過10GPa且為15GPa以下
D 超過15GPa
將包含依上述之順序所得之樹脂組成物的溶液塗佈在塑膠基材(實施脫模處理之PET薄膜)的單面,於100℃乾燥5分鐘。藉此,製作厚度約100μm之薄片。藉由層合4枚製作之薄片在200℃、5MPa的條件,沖壓60分鐘使其硬化,而得到樹脂硬化物。將此切出10mm×10mm。使用熱傳導率測定裝置(LFA447 NanoFlash、NETZSCH公司製),進行在經切出之樹脂硬化物的熱傳導率的測定。
將包含依上述之順序所得之樹脂組成物的溶液塗佈在塑膠基材(實施脫模處理之PET薄膜)的單面,於100℃乾燥5分鐘。藉此,製作厚度約100μm之薄片。將製作之薄片挾在厚度70μm之銅箔(CF-T8G-THE-70(商品名)、福田金屬箔粉工業股份有限公司製)的粗糙化面之間,在200℃、5MPa的條件,沖壓60分鐘。將沖壓之試驗片切斷成10mm
寬。使用被切斷之試驗片,在autograph,在剝離角度180度,測定剝離銅箔時之接著力。
將所得之結果以下述基準評估。
A 25N/10mm以上
B 15N/10mm以上且未滿25N/10mm
C 未滿15N/10mm
將包含依上述之順序所得之樹脂組成物的溶液塗佈在塑膠基材(實施脫模處理之PET薄膜)的單面,於100℃乾燥5分鐘。藉此,製作厚度約100μm之薄片。將製作之薄片挾在厚度18μm之銅(CF-T9FZ-SV-18(商品名)、福田金屬箔粉工業股份有限公司製)的粗糙化面之間,在200℃、5MPa的條件,沖壓60分鐘。將沖壓之試驗片切斷成25mm×25mm。將被切斷之試驗片於280℃及300℃之焊料浴漂浮3分鐘。然後,進行確認是否發生膨脹(3分鐘膨脹)。
將所得之結果以下述基準評估。
A 在300℃ 3分鐘無膨脹
B 在280℃ 3分鐘無膨脹
C 在280℃於3分鐘以內發生膨脹
將結果示於下述表。
於實施例1~13,任一者皆為於-40℃之儲藏彈性率為15GPa以下,熱傳導率為2W/m.K以上,70μm銅箔接著力為15N/10mm以上。又,於焊接耐熱性評估,達成280℃ 3min。尚,於實施例1~13之組成任一皆為於23℃之儲藏彈性率為5GPa以下。
尚,實施例2相對於實施例1,係進一步添加(E)成分之硬化觸媒之實施例。實施例3相對於實施例2,係變更(D)成分之無機填料及(E)成分之硬化觸媒的摻合比例之實施例。實施例4相對於實施例1,係變更(B)成分之溶劑可溶性聚醯亞胺的種類之實施例。實施例5相對於實施例2,係作為(D)成分之無機填料,併用鱗片狀氮化硼,且變更(D)成分之無機填料的摻合比例之實施例。實施例6相對於
實施例1,作為(D)成分之無機填料,併用凝聚氮化硼,且變更(D)成分之無機填料的摻合比例之實施例。實施例7及10相對於實施例1,係變更(A)成分之具有酸酐基之改質彈性體、(B)成分之溶劑可溶性聚醯亞胺及(C)成分之環氧樹脂的摻合比例之實施例。實施例8、9、12及13相對於實施例1,係變更(A)成分之具有酸酐基之改質彈性體及(B)成分之溶劑可溶性聚醯亞胺的摻合比例之實施例。實施例11相對於實施例1,係變更(A)成分之具有酸酐基之改質彈性體的種類之實施例。
比較例1係未摻合(B)成分之溶劑可溶性聚醯亞胺之比較例。於比較例1,在焊接耐熱性評估所得之數值未滿280℃ 3min。比較例2係未摻合(C)成分之環氧樹脂之比較例。於比較例2,在焊接耐熱性評估所得之數值未滿280℃ 3min。比較例3係取代(A)成分之具有酸酐基之改質彈性體,改摻合無馬來酸改質之苯乙烯系彈性體之比較例。於比較例3,70μm銅箔接著力未滿15N/10mm,且在焊接耐熱性評估所得之數值未滿280℃ 3min。比較例4係未摻合(A)成分之具有酸酐基之改質彈性體之比較例。於比較例4,於-40℃之儲藏彈性率超過15GPa,且在焊接耐熱性評估所得之數值未滿280℃ 3min。
Claims (9)
- 一種樹脂組成物,其特徵為包含(A)具有酸酐基之改質彈性體、(B)溶劑可溶性聚醯亞胺樹脂及(C)環氧樹脂,前述(A)的含量,以相對於前述(A)、前述(B)及前述(C)之合計的固體成分質量的質量%計為40質量%以上,前述(B)成分的含量,相對於(A)成分、(B)成分及(C)成分之合計的固體成分質量,以質量%為1~45%,前述(C)成分的含量相對於(A)成分、(B)成分及(C)成分之合計的固體成分質量,以質量%為1%以上。
- 如請求項1之樹脂組成物,其中,前述(A)為被馬來酸酐改質之苯乙烯系彈性體。
- 如請求項1或2之樹脂組成物,其中,前述(B)為使四羧酸成分、與二聚物二胺反應所得之聚醯亞胺樹脂。
- 如請求項1或2之樹脂組成物,其係進一步含有(D)無機填料。
- 如請求項4之樹脂組成物,其中,前述(D)為具有10W/m.K以上之熱傳導率的熱傳導性填料。
- 一種附基材薄膜,其係包含塑膠基材、與形成在前述塑膠基材的至少一面之由如請求項1~5中任一項之樹脂組成物而成之層。
- 一種金屬/樹脂層合物,其係包含金屬板或金屬箔、與形成在前述金屬板或金屬箔的至少一面之由如請求項1~5中任一項之樹脂組成物而成之層。
- 一種樹脂硬化物,其係如請求項1~5中任一項之樹脂組成物的硬化物。
- 一種使用如請求項1~5中任一項之樹脂組成物的半導體裝置。
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