TW528775B - High dielectric constant flexible polyimide film and process of preparation - Google Patents
High dielectric constant flexible polyimide film and process of preparation Download PDFInfo
- Publication number
- TW528775B TW528775B TW87109894A TW87109894A TW528775B TW 528775 B TW528775 B TW 528775B TW 87109894 A TW87109894 A TW 87109894A TW 87109894 A TW87109894 A TW 87109894A TW 528775 B TW528775 B TW 528775B
- Authority
- TW
- Taiwan
- Prior art keywords
- dielectric constant
- ceramic magnetic
- magnetic filler
- film
- polyimide
- Prior art date
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- 229920001721 polyimide Polymers 0.000 title claims abstract description 101
- 238000000034 method Methods 0.000 title claims description 9
- 238000002360 preparation method Methods 0.000 title description 2
- 239000000919 ceramic Substances 0.000 claims abstract description 90
- 239000010410 layer Substances 0.000 claims abstract description 61
- 229910002113 barium titanate Inorganic materials 0.000 claims abstract description 50
- 239000004642 Polyimide Substances 0.000 claims abstract description 49
- JRPBQTZRNDNNOP-UHFFFAOYSA-N barium titanate Chemical compound [Ba+2].[Ba+2].[O-][Ti]([O-])([O-])[O-] JRPBQTZRNDNNOP-UHFFFAOYSA-N 0.000 claims abstract description 44
- 230000001070 adhesive effect Effects 0.000 claims abstract description 32
- 239000000853 adhesive Substances 0.000 claims abstract description 31
- 239000000945 filler Substances 0.000 claims abstract description 30
- 229920006259 thermoplastic polyimide Polymers 0.000 claims abstract description 24
- 239000002356 single layer Substances 0.000 claims abstract description 14
- 239000012762 magnetic filler Substances 0.000 claims description 73
- 229920002098 polyfluorene Polymers 0.000 claims description 40
- GTDPSWPPOUPBNX-UHFFFAOYSA-N ac1mqpva Chemical compound CC12C(=O)OC(=O)C1(C)C1(C)C2(C)C(=O)OC1=O GTDPSWPPOUPBNX-UHFFFAOYSA-N 0.000 claims description 39
- 150000003949 imides Chemical class 0.000 claims description 32
- 229920001169 thermoplastic Polymers 0.000 claims description 29
- 239000004416 thermosoftening plastic Substances 0.000 claims description 29
- -1 aromatic ether diamine Chemical class 0.000 claims description 28
- 229920001187 thermosetting polymer Polymers 0.000 claims description 25
- VLDPXPPHXDGHEW-UHFFFAOYSA-N 1-chloro-2-dichlorophosphoryloxybenzene Chemical compound ClC1=CC=CC=C1OP(Cl)(Cl)=O VLDPXPPHXDGHEW-UHFFFAOYSA-N 0.000 claims description 24
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 claims description 21
- 150000002466 imines Chemical group 0.000 claims description 21
- 239000002253 acid Substances 0.000 claims description 19
- 239000000203 mixture Substances 0.000 claims description 18
- 239000002245 particle Substances 0.000 claims description 17
- 239000007788 liquid Substances 0.000 claims description 14
- 125000004432 carbon atom Chemical group C* 0.000 claims description 11
- NIHNNTQXNPWCJQ-UHFFFAOYSA-N o-biphenylenemethane Natural products C1=CC=C2CC3=CC=CC=C3C2=C1 NIHNNTQXNPWCJQ-UHFFFAOYSA-N 0.000 claims description 11
- 229920005575 poly(amic acid) Polymers 0.000 claims description 11
- 125000003118 aryl group Chemical group 0.000 claims description 10
- 150000004985 diamines Chemical class 0.000 claims description 10
- 239000000126 substance Substances 0.000 claims description 10
- CYIDZMCFTVVTJO-UHFFFAOYSA-N pyromellityc acid Natural products OC(=O)C1=CC(C(O)=O)=C(C(O)=O)C=C1C(O)=O CYIDZMCFTVVTJO-UHFFFAOYSA-N 0.000 claims description 9
- WUPRYUDHUFLKFL-UHFFFAOYSA-N 4-[3-(4-aminophenoxy)phenoxy]aniline Chemical compound C1=CC(N)=CC=C1OC1=CC=CC(OC=2C=CC(N)=CC=2)=C1 WUPRYUDHUFLKFL-UHFFFAOYSA-N 0.000 claims description 8
- 229910052799 carbon Inorganic materials 0.000 claims description 8
- NAQMVNRVTILPCV-UHFFFAOYSA-N hexane-1,6-diamine Chemical compound NCCCCCCN NAQMVNRVTILPCV-UHFFFAOYSA-N 0.000 claims description 8
- HLBLWEWZXPIGSM-UHFFFAOYSA-N 4-Aminophenyl ether Chemical compound C1=CC(N)=CC=C1OC1=CC=C(N)C=C1 HLBLWEWZXPIGSM-UHFFFAOYSA-N 0.000 claims description 7
- 238000000576 coating method Methods 0.000 claims description 7
- 125000003277 amino group Chemical group 0.000 claims description 6
- RYYUUQPLFHRZOY-UHFFFAOYSA-N 4-[2-(4-aminophenoxy)phenoxy]aniline Chemical compound C1=CC(N)=CC=C1OC1=CC=CC=C1OC1=CC=C(N)C=C1 RYYUUQPLFHRZOY-UHFFFAOYSA-N 0.000 claims description 5
- JVERADGGGBYHNP-UHFFFAOYSA-N 5-phenylbenzene-1,2,3,4-tetracarboxylic acid Chemical compound OC(=O)C1=C(C(O)=O)C(C(=O)O)=CC(C=2C=CC=CC=2)=C1C(O)=O JVERADGGGBYHNP-UHFFFAOYSA-N 0.000 claims description 5
- 229910052788 barium Inorganic materials 0.000 claims description 5
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- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 4
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- PCTMTFRHKVHKIS-BMFZQQSSSA-N (1s,3r,4e,6e,8e,10e,12e,14e,16e,18s,19r,20r,21s,25r,27r,30r,31r,33s,35r,37s,38r)-3-[(2r,3s,4s,5s,6r)-4-amino-3,5-dihydroxy-6-methyloxan-2-yl]oxy-19,25,27,30,31,33,35,37-octahydroxy-18,20,21-trimethyl-23-oxo-22,39-dioxabicyclo[33.3.1]nonatriaconta-4,6,8,10 Chemical compound C1C=C2C[C@@H](OS(O)(=O)=O)CC[C@]2(C)[C@@H]2[C@@H]1[C@@H]1CC[C@H]([C@H](C)CCCC(C)C)[C@@]1(C)CC2.O[C@H]1[C@@H](N)[C@H](O)[C@@H](C)O[C@H]1O[C@H]1/C=C/C=C/C=C/C=C/C=C/C=C/C=C/[C@H](C)[C@@H](O)[C@@H](C)[C@H](C)OC(=O)C[C@H](O)C[C@H](O)CC[C@@H](O)[C@H](O)C[C@H](O)C[C@](O)(C[C@H](O)[C@H]2C(O)=O)O[C@H]2C1 PCTMTFRHKVHKIS-BMFZQQSSSA-N 0.000 claims 3
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 claims 3
- LGRFSURHDFAFJT-UHFFFAOYSA-N Phthalic anhydride Natural products C1=CC=C2C(=O)OC(=O)C2=C1 LGRFSURHDFAFJT-UHFFFAOYSA-N 0.000 claims 2
- JHIWVOJDXOSYLW-UHFFFAOYSA-N butyl 2,2-difluorocyclopropane-1-carboxylate Chemical compound CCCCOC(=O)C1CC1(F)F JHIWVOJDXOSYLW-UHFFFAOYSA-N 0.000 claims 2
- 238000012856 packing Methods 0.000 claims 2
- DWMXTYHQOUAVCW-UHFFFAOYSA-N 1,2-diphenyl-9H-fluoren-3-amine Chemical compound NC=1C(=C(C=2CC3=CC=CC=C3C=2C=1)C1=CC=CC=C1)C1=CC=CC=C1 DWMXTYHQOUAVCW-UHFFFAOYSA-N 0.000 claims 1
- TWKVCLRLFUIZLG-UHFFFAOYSA-N 5-(4-carboxyphenyl)cyclohexa-2,4-diene-1,1,2-tricarboxylic acid Chemical compound C1C(C(O)=O)(C(O)=O)C(C(=O)O)=CC=C1C1=CC=C(C(O)=O)C=C1 TWKVCLRLFUIZLG-UHFFFAOYSA-N 0.000 claims 1
- 229910017619 MgSn Inorganic materials 0.000 claims 1
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- 229910004413 SrSn Inorganic materials 0.000 claims 1
- 150000008064 anhydrides Chemical class 0.000 claims 1
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- GCAIEATUVJFSMC-UHFFFAOYSA-N benzene-1,2,3,4-tetracarboxylic acid Chemical compound OC(=O)C1=CC=C(C(O)=O)C(C(O)=O)=C1C(O)=O GCAIEATUVJFSMC-UHFFFAOYSA-N 0.000 claims 1
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- USIUVYZYUHIAEV-UHFFFAOYSA-N diphenyl ether Chemical compound C=1C=CC=CC=1OC1=CC=CC=C1 USIUVYZYUHIAEV-UHFFFAOYSA-N 0.000 claims 1
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- OLAPPGSPBNVTRF-UHFFFAOYSA-N naphthalene-1,4,5,8-tetracarboxylic acid Chemical compound C1=CC(C(O)=O)=C2C(C(=O)O)=CC=C(C(O)=O)C2=C1C(O)=O OLAPPGSPBNVTRF-UHFFFAOYSA-N 0.000 claims 1
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- 229920003223 poly(pyromellitimide-1,4-diphenyl ether) Polymers 0.000 description 8
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- H05K2201/0335—Layered conductors or foils
- H05K2201/0355—Metal foils
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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
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- H05K2201/09309—Core having two or more power planes; Capacitive laminate of two power planes
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- H—ELECTRICITY
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- H05K3/00—Apparatus or processes for manufacturing printed circuits
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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
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
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- Chemical Kinetics & Catalysis (AREA)
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- Compositions Of Macromolecular Compounds (AREA)
Description
峨775
發明説明（ Ψ 遊 發明背景 本發明係有關於一種撓性高介 (讀先閱讀背面之注意事項再填寫本頁) 人铷乃古人不 思吊數氷酿亞胺薄膜，複 其可用於電子電路及電 薄膜層印刷電路，繞性電路，半導體封裝及埋置 告習用去輕電容器係裝在印刷電路板之表面上，並連接至 非近集成電路之電源及接地面。就具有大量集成電路之血 型印刷電路板而言，一般需要相對 /、 w耵大里心去耦電客器來提 、包流需求及降低系統嗓音。然而，此等電容器有其缺 ·=:因馬彼等將占據相當大的印刷電路板表面空間，增加 焊接點之數量，而因此降低系統之可靠度。 g 經濟部中央標準局員工消費合作社印t 最近，已發展出新式電容器設計，稱爲埋置薄膜電容 為，其可產生充足旁路電容，由印刷電路板全體共用。例 如，美國專利5，162,977號（1992年11月1〇日頒予1^111.旧等 人）揭示一種印刷電路板，其包括嵌入之高電容功率分佈 芯，該芯係由信號接地面與電源面，藉由具有高介電常數 之介電芯元件隔開所組成。此埋置電容結構不僅提供電磁 干擾（Ε ΜI)抑制，而且可自印刷電路板除去高達9 8 %之分 立旁路電容器。美國專利5,162,977號所揭示的介電芯元件 係由玻璃布浸滿環氧樹脂，而環氧樹脂中加具高介電常數 之鐵電陶資粉所組成。然而，此種玻璃纖維浸滿環氧街月匕 之系統提供之電容密度雖可高達2000微微法拉/平方叶 (Picofarads/in2)，但其並不足以應付大多數集成電路之 湧入電流需求。 -4 本纸張尺度適用中國國家標準（CNS ) A4規格（210X297公釐） 528775 A7 B7 五、 發明説明（ 2 f 本發明提供-種呈薄膜，複合或液體型之撓性高介電常 數聚醯亞胺，其在印刷電路板或半導體封裝中作爲嵌2高 電容功率分佈芯之介電芯組件使用時，由於可得之介電常 數更高及所用之薄膜結構更薄，故可提供更高之電二:面 密度，達200,000微微法拉/平方吋。具有此等電徵之 印刷電路板對相聯之印刷電路板組件一般不需要額外i去 耦，因此可免用裝在印刷電路板外部之去耦電容器。 發明概述 本發明提供一種高介電常數撓性聚醯亞胺薄膜，其包含 單一層之黏著性熱塑性聚醯亞胺薄膜，其中分散著4_85; 里％ (以薄膜重f爲準）之鐵電陶磁塡料；其中聚醯亞胺薄 膜之介電常數爲4-60。 本發明也提供一種高介電常數聚醯亞胺液體，其包含工至 3 0重量％熱塑性或熱固性聚醯胺酸溶於丨〇至9 5重量％惰性 有機溶劑’其中分散著4-90重量％鐵電陶磁填料：且具介 電常數爲4-300。 經漓部中央標準局員工消費合作社印1ί (請先閱讀背面之注意事項再填寫本育)
、1T 本發明進一步提供一種高介電常數撓性多層聚醯亞胺薄 膜，其包含中間熱塑性或熱固性聚醯亞胺薄膜層，其—面 或兩面具有薄層之熱塑性聚醯亞胺薄膜，且至少一聚鱗亞 胺層中分散有4-85重量％(以薄膜層重量爲準）之鐵電陶磁 填料；其中多層聚酿亞胺薄膜之介電常數爲4-60。 本發明進一步提供一種印刷電路板，其包括嵌入高電容 功率分佈芯，該芯包含： (a)導電接地面層： 5 本紙張尺度適用中國國家標準（CNS ) A4規格（210X297公釐） 528775 五 、發明説明（ 3 A7 B7 -------— (b )導電電源面層：及 高係配置於該接地面層與該電源面層間之撓性 ^ "牛，其包含早一層之黏著性熱塑性聚醯亞胺蘇 ,或多層聚醯亞胺薄膜，該多層聚醯亞胺薄膜包含—中間 =性或熱固性聚酿亞胺薄膜層，其_面或兩面^ ^ :“鉍亞胺薄膜，且至少-層聚醯亞胺薄膜層 :刀政有心85重量％(以薄膜層重量爲準)之鐵電陶磁塡 料’及其中薄膜之介電常數爲4-60。 發明之詳細説明 本發明係有關於一種撓性高介電常數聚醯亞胺薄膜，其 係由單層之黏著性熱塑性聚醯亞胺薄膜，或薄膜之一面或 兩面粘$黏著性熱塑性聚酸亞胺薄膜層並含有高介電常數 鐵電陶磁填料或填料混合物之多層聚醯亞胺薄膜所構成。 黏著性熱塑性聚醯亞胺薄膜層可提供對各種金屬基質如 電容器接地及電源面之附著力，並提供更平滑表面以增加 有效電容面積。 本發明所用之黏著性熱塑性聚驢亞胺薄膜包括環氧化 物’丙烯酸，聚氨基甲酸酯及聚醯亞胺薄膜。特佳者爲熱 可溶封，熱塑性，無規或嵌段聚醯亞胺，其含有6 〇至9 8莫 耳％ ’較佳7 0至9 5莫耳。/〇由4，4，_氧苯二酸二酐及具以下化 學式之芳族醚二胺所衍生之重複醯亞胺單元
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-6- 本紙張尺度適用中國國家標準（CNS ) A4規格（210X297公釐） (請先閱讀背面之注意事項再填寫本頁} 經濟部中央標率局員工消費合作社印製
A 528775 A7 B7 五、發明説明（4 及2至4 0莫耳％，較佳2至2 5莫耳〇/ + ^ a ^ -TL 夭吁/。由四價芳族羧酸二酐及 具以下化學式之二價脂族或苦放一 飞万狹—胺所衍生之額外重複酿 亞胺單元
on CN πο^/R、OMC^ VMMO (讀先閱讀背面之注意事項再填寫本頁j % 其中R爲芳族四價有機基及Rl爲含有至少2個麵子 或脂族二胺之二價基，二胺之二個氨基各附於 之= 別碳原子。 情卷 < 個 代表性芳族醚二胺包括： i，2_雙（4-氨基苯氧基）苯 I 3 -雙（4 -氨基苯氧基）苯 12-雙（3-氨基苯氧基）苯 1 3 -雙（3·氨基苯氧基）苯 le(4 -氨基苯氧基）-3-(3_氨基苯氧基）苯 1，4 -雙（4 -氣基苯氧基）苯 14-雙（3·氨基苯氧基）苯 1-(4-氨基苯氧基）-4-(3_氨基苯氧基）苯 此等額外醯亞胺單元可自與先前定義之4,4，_氧苯二酸一 纤及芳族醚二胺相同或不同之二酐及二胺衍生。 表紙張尺度適用中國國家標準（CNS ) A4規格（2丨0X297公釐） -訂 經滴部中央標準局員工消費合作社印掣 528775 A7 B7 五、發明説明（5 ) 特佳之二酐及二胺包括下列·· 苯均四酸二酐： 4，4 ’ -氧苯二酸二酐： 3,3’，4,4’-二苯甲酮四羧酸二酐： 2,2’，3,3’ -二苯甲酮四羧酸二酐： 3,3 ’，4，4 ’ -聯苯四羧酸二酐： 2，2 ’，3,3 · ·聯苯四羧酸二酐： 2.2 -雙（3,4 -二羧基苯基）六氟丙烷二酐： 雙（3,4-二羧基苯基）颯二酐； 雙（3,4-二羧基苯基）硫化二酐： 雙（2，3 -二羧基苯基）甲烷二酐； 雙（3,4 -二羧基苯基）甲烷二酐； 1.1- 雙（2,3 -二羧基苯基）乙烷二酐： 1.1- 雙（2,3 -二羧基苯基）丙烷二酐： 2,2_雙（3,4 -二羧基苯基）丙烷二酐： 間-伸苯基雙（苯偏三酸）二酐： 六亞甲二胺： 七亞甲二胺： 3.3 -二甲基五亞甲二胺： 經濟部中央標率局員_x消費合竹社印策 (請先閱讀背面之注意事項再填寫本頁) 3 -甲基六亞甲二胺： 3 -甲基七亞甲二胺： 2,5 -二甲基六亞甲二胺： 八亞甲二胺： 九亞甲二胺： 1,1,6,6 -四甲基六亞甲二胺： _1_§_1_ 本紙張尺度適用中國國家標準（CNS ) A4規格（210X 公釐） 528775 A7 B7 五、發明説明（6 ) 2,2,5,5 -四甲基六亞甲二胺： 4,4 -二甲基七亞甲二胺： 十亞甲二胺： 間-冬—胺； 4，4’ -二氨基二苯甲酮： 4 _氨基苯基-3 -氨基甲酸酯； 間-氨基苯醯基-對·氨基醯替苯胺； 4，4 ’ - —基二木基酸； 3,4’-二氨基二苯基醚： 雙（4·氨基苯基）甲烷： 1，1 -雙（4 -氨基苯基）乙烷： 2.2- 雙（4-氨基苯基）丙烷： 4，4 ’ -二氣基二木基亞諷； 3,3’-二氨基二苯甲酮： 1，3 -雙（4 -氣基苯氧基）苯； 2，2’ -二氨基二苯甲酮： 1.2- 雙（4-氨基苯氧基）苯： 1，3 -雙（4 -氣基苯氧基）苯： 經滴部中央標率局員工消費合作社印製 (讀先閱讀背面之注意事項再填寫本頁) 4,4、二氨基苯醯替苯胺； 4,4’-雙（4-氨基苯氧基）苯基醚： 2，2 ’ -雙（4 -氨基苯基）六氟丙烷： 2,2’ -雙（4_氨基苯基）·1，3·二氯-1,1,3,3 -四氟丙烷： 4，4f -二氨基二苯基諷： 1，12 -二氨基十二烷：及 -9- 本纸張尺度適用中國國家標準（CNS ) A4規格（210X297公釐） 528775 A7 B7 經漓部中央標準局員工消費合作社印繁 五、發明説明（7 ) 1，1 3 -二氨基十三'j：兔。 用於本發明之適當黏著性熱塑性聚醯亞胺已揭示於美國 專利5,298,3；5 1號（I"4年3月29日頒予雄n等人）， 其揭示内客併於此以供參考。 用於本發明之特佳黏著性聚醯亞胺含有7 〇至9 5莫耳％ 4,4’-氧苯二酸二酐，5至3〇莫耳％苯均四酸二酐及1〇〇莫 耳％1，〕-雙（4-氨基苯氧基）苯，及8〇至95莫耳％1,3-雙 (4 -氨基苯氧基）苯’ 5至20莫耳％六亞甲二胺及1〇〇莫耳％ 4,4’-氧苯二酸二酐^ 由j，*? , 4，4 -聯苯基四幾酸二肝（BpDA )，苯均四酸二奸 (PMD A )及4，4 ’ _二氨基二苯基醚衍生之熱塑性聚醯亞胺也 可用作爲爲聚_亞胺薄膜黏著性層。BPDA比PMDA之範圍 爲0.3 : 0.7，以55/45 BPDA/PMDA共聚物薄膜爲較佳。 可用於本發明之鐵電陶磁填料之較佳實例包括具粒度自 0· 10至1 0微米及具高介電常數自1〇〇至3〇 〇〇〇之微粒鐵電 陶磁粉末。 陶磁填料之特定實例包括BaTi〇3，SrTi〇3，Mg2Tic^，
Bi2(Ti03)3，PbTi〇3，NiTi03，CaTi03，ZnTi03，
Zn2Ti04，BaSn03，Bi(Sn03)3，CaSn03，pbSn03， MgSn03，SrSnO;，ZnSn03，BaZrO;，CaZr〇3，PbZr03，
MgZn〇3, SrZr〇3及ZnZr〇3。密實多結晶陶磁，如鈦酸鋇及 錘酸鉛，用於本發明特佳。 總介電常數之改進係藉併入其量爲4 - 8 5重量％，較佳2 〇 至7 5重量％(以薄膜組合物之總重爲準）之陶磁填料而得。 陶磁填料在4重量％以下不會提供必要的介電常數，而陶磁 -10- 本紙張尺度適用中國國家標準（CNS ) A4規格（210X297公釐） (請先閱讀背面之注意事項再填寫本頁) 、-口 528775 Α7 Β7 五、發明説明（8 ) '一·' -- 填料含量在8 5重量％以卜目，丨見太_ 上/、】易使浔膜機械性皙降級。含有 2 0至6 5重量％陶磁塡料— (讀先閱讀背面之注意事項再填寫本頁} 、十尤其疋可提供介電常數1 0至2 7 I鈦酸鋇一之薄膜可獲得特別好的結果。 陶磁粉末填料可個別俅〜 _ 使用而獲仔艮好效果。然而，當彼 寺以適當組合使用時，介雷赍* 1私吊數 < 改進可達到甚至更大程 度。 例如’鈇酸鋇係-種商業產品，可獲得各種等級，其特 ，馬介電常數自約100至30，_。鈦酸鋇之介電常數，如所 热知，在居里點時達到最大。不用1〇〇 %之單一鈦酸鋇，可 用具不同居里點之鈦酸鹽之組合來維持以溫度爲函數之恆 定介電性能。 陶磁填料如鈦酸鋇與導電皮/芯微粒填料之混合物也可 用以提高介電常數。此等導電皮/芯填料包括Zelec@ Ecp 3005-XC，市面上可自杜邦公司購得。Zelec@ Ec：p 3〇〇5_ XC係一種經摻雜銻之氧化錫塗覆之矽氧粒子填料，含有 6.5/。綈，〇50粒度爲〇7微米。5至80重量％鈥酸鋇與5至 15重量％ Zelec® ECp 3〇〇5-XC之混合物可提供具有介電常 數5至6 0之薄膜，其具良好伸長率及黏著性質。 經滴部中央標準局員工消費合作社印餐 爲獲得良好薄膜完整性及甚至更高介電常數，陶磁填料 也可在分散於聚醯亞胺基質之前，先以聚醯亞胺塗覆表 面。聚酸亞胺基質可爲先前所述熱塑性聚醯亞胺，或如由 苯均四酸二酐與4,4，-二氨基二苯基醚反應製備之熱固性聚 驢亞胺。填料之聚醯亞胺表面可提供物理及化學黏合部 位，例如，-N Η2，- 0 ( C 0 )2，以使聚醯亞胺基質黏合於 -11 -
丁 - I I 528775 A7 B7 經濟部中央標率局員Η消費合作衽印聚 五、發明説明（9 G料得到更佳之薄膜機械性質。此外，經聚醯亞胺塗覆 之:料可在磁_料表面提供均勾聚合物塗層，防止填料 视=〈而形成聚合物-填料網絡，因此提高介電常數及可能 之W料最大3 !水準。在典型實例中，經7重量。/❶聚醯胺 (&由苯均四I —酐及4，4 二氨基二苯基醚衍生者）塗覆之鈦 酉欠鎖％料’其使用之最大含量爲7 5重量％，而未塗覆之鈦 酸鎖填料’其使用之最大填料含量爲60重量％。介電常數 相應地由未塗覆鈦酸鋇之丨3增高至經聚醯亞胺塗層之鈦酸 鋇之3 5。 、聚醯亞胺表面塗層可含有1至99重量，較佳3至40重量％ •^經塗覆陶磁填料，如鈦酸鋇，而提供具有介電常數3至 之薄膜氷®益亞胺表面塗層之厚度自10毫微米至20毫 微米，較佳自3〇〇毫微米至3微米。 I醞亞胺表面塗層包括由苯均四酸二酐（pMDA )與4，*，· 二氨基二苯基醚：4,4、氧苯二酸二酐（〇DpA)，苯均四酸 2酐（PMDA)與丨，3-雙（4-氨基苯氧基）苯：及3,3，，4,4，_聯 苯四羧鉍二酐（BPDA)，苯均四酸二酐（pMDA)與4,4，·二 氨基二苯基醚所形成之聚醯亞胺。 經聚醯亞胺塗覆之陶磁填料可單獨使用或與未塗覆陶磁 ，料混合使用。40至60重量％未塗覆鈦酸鋇與6〇至4〇重 f %經7重量％聚醯亞胺塗覆之鈦酸鋇所形成之混合物可提 供最小填料凝聚，並提高聚醯亞胺薄膜之介電常數自2〇至 35 〇 高介電常數聚醯亞胺薄膜或複合物可藉將表面已塗覆聚 -------- 衣-------II (讀先閱讀背面之注意事項再填寫本頁)
528775 A7 B7 經滴部中央標準局員工消費合作社印製 五、發明説明（10) 醯胺酸之陶磁填料，不必使用聚醯亞胺基質，熔體擠壓/ 或壓縮成薄片或三維度複合物而製備。 塗覆在陶磁填料表面之聚醯胺酸可爲黏著性熱塑性或熱 固性聚醯胺酸，如〇DP A/ PMDA/丨，％雙（4_氨基苯氧基） 苯：ODP A /六亞甲二胺/】，3_雙（心氨基苯氧基）苯； BPDA/PMDA /44-二氨基二苯基醚；及 pMDA/4 4•二 氨基二苯基醚。陶磁填料可爲先前所述任何一種，尤其是 鈦酸鋇。以典型實例言之，由表面塗覆8至40重量％聚醯 胺酸t鈦酸鋇填料製備之熱壓縮聚醯亞胺，據測量，具有 介電常數爲15至！7〇。 ' 问介電常數陶磁填料之併入聚醯亞胺薄膜中係如下進 行：將陶磁塡料粉碎或粒度自〇1〇至1〇微米之粒子，將粒 子和聚醯胺酸前驅聚合物之溶液混合及將所得混合物用^ 知落劑模鑄造扶術鑄造成薄膜形狀。 本發明<鬲介電常數聚醯亞胺薄膜可形成爲單一層或多 層構造。除非所製得之薄膜含有至少4重量％，較佳至少 2 〇重量❶/° (以單層或多層聚醯亞胺薄膜總重爲準）之陶磁壚 料，否則介電常數得不到明顯的改良。 ” a作馬形成多層構造之方式，可使用的有擠壓-層合方法， 熱壓縮f法，溶液塗覆法及共擠壓法。這些都是可用於开, 成夕層薄膜之方法之典型，但非全部之實例。 —爲提高—多層聚醯亞胺薄膜—中間熱塑性或熱固性聚醯 胺g，薄Λ塑性黏著性聚醯亞胺外層所組成者—之介電常 數，高介電常數陶磁填料必須併入多層結構之至少一= 本紙張尺度適用中公釐)-^ I 11 衣 11, n I n ϋ、π - - (請先閲讀背面之注意事項再填寫本頁} 528775 經滴部中决標準局負工消費合作社印$1 Α7 Β7 五、發明説明（11 ) 4 0至7 5重量0/〇之陶磁填料可併入中間聚醯亞胺層以提供多 層結構介電常數自6至24。陶磁填料也可併入外薄黏著性 聚醯亞胺層中以進一步提高介電常數。然而，併入薄黏著 性聚酿亞胺層及中間聚醯亞胺之陶磁填料濃度必須加以調 整以使最終多層聚臨:亞胺薄膜之物理性質及黏著剥離強度 最大化。一般可將20至50重量％之陶磁填料併入外黏著性 聚醯亞胺層之每一層中。 多層薄膜結構之總厚度爲自5至125微米。中間聚醯亞胺 層之厚度爲自5至120微米，而外黏著性聚醯亞胺層之厚度 則爲5至6 0微米。 多層結構的中間聚醯亞胺層可爲先前所述類型之熱塑性 聚醯亞胺，或熱固性聚醯亞胺如Kapt〇n®一由苯均四酸二酐 與4，4 -二氨基二苯基醚衍生而得，市面上可自杜邦公司購 得。 聚醯亞胺共聚物薄膜，如由3,3，，4,4，-聯苯四羧酸二酐 (BPDA)，苯均四酸二酐（PMDA)及4,4，_二氨基二苯基 醚，含有5 5 /45莫耳比BPDA/PmDA所衍生者；以及3〇 至50莫耳％〇卩〇八，50至70莫耳％卩]^人，60至80莫耳％ 對-苯二胺及2 〇至4 〇莫耳％4，4，-二氨基二苯基醚所衍生之 共聚酿亞胺薄膜都可用作爲中間聚醯亞胺層。 知薄膜形成多層構造而非單層構造之優點爲陶磁填料會 在單層薄膜之表面上形成不規則性，故當薄膜和銅箔疊置 形成電容器時，空氣會陷在介面中至一定程度而降低總介 電常數。此種非所欲現象可藉將薄膜形成由中間聚醯亞胺 -14- 本紙張尺度通用宁國國家標準（CNS ) A4規格（210χ297公釐 (請先閱讀背面之注意事項再填寫本頁) ，11 )28775 五、發明説明（12 A7 B7 經濟部中央標準局員工消費合作社印製 二人=，奢性聚酿亞胺薄外層所組成的多層構造而排 2。在此種，層構造中，由於陶磁填料粒子之過高含量而 現在反面之可能不良影響，可藉由含有陶磁填料粒 表：二外Γ著性聚酿亞胺層而實質消除。所得更平滑的 表面可增加有效電容面積。 、本發介電常數撓性_亞料膜可料電子電路界r多用途上。例如，聚"亞胺薄膜可用： ^寸时封农及印刷線路板封裝之埋置薄膜電容器。 半導體封裝料時，聚醯亞胺薄膜基質之總電容 兩求較印刷電路板用途所需者高出很多（>⑽倍）。電容密 ’又與’I包：數直接成正比，而與基質之厚度成反比。電容 之增強可藉提高介電常數或降低經陶磁填充之介電層之厚度而達成。 :已發現，Μ陶磁填充之熱塑性聚酸亞胺液體可藉習用方 _旋塗賣塗，幕塗等薄之直接施塗於導體面。薄層之 阿）丨屯¥數聚醯胺酸液體接著可藉熱及/或化學及/或光 處:里丁以烘乾及硬化而成薄聚醯亞胺層。由於能形成厚度 2 5微米之薄聚醯亞胺層，故使用聚醯胺酸液體將使電 奋2使用相同楱料含量水準之自立聚醯亞胺薄膜增加1 〇倍 =夕。此外，使用聚醯胺酸液體較之自立聚醯亞胺薄膜可 知更呵重里陶磁填料含量（高達9〇重量，因爲對薄 膜f理完整性較無須限制。以典型實例言之，使㈤含有9〇 重量％陶磁填料之聚醯胺酸液體可得17〇之高介電常數。 本發明現將參照以下工作實例及比較實例更明確加以説
(讀先閱讀背面之注意事項再填寫本頁) 訂 f 528775 A7 B7 13 五、發明説明（ 明。然而，本發明無論如何不受以下實例限制。 使用以下標準ASTM試驗方法測量實例中所述之薄膜性 質： 介電常數（MHz) —ASTM No· D-150 伸長率（％) —ASTM No. D-882 剥離強度（psi) — ASTM No. D-5109 抗張強度（Kpsi) —ASTM No. D-882 模量（Kpsi) —ASTM No· D-882 電容（Pfarads/in2) —ASTM No. D-150 J 黾強度（V / 〇nil) — ASTM No. D-149 實例1至9 (比較實例1 C ) 實例1至9將說明本發明單層黏著性熱塑性聚醯亞胺薄膜 以鈥酸鋇填料用量由1 5增加至7 3重量％ (以薄膜總重爲準） 爲函數之介電常數之增加。30至63重量％之最適量鈦酸鋇 填料提供之介電常數高達10至27，而與不含鈦酸鋇填料之 實例1 C比較，仍維持良好薄膜伸長率及抗張強度。 (請先閱讀背面之注意事項再填寫本頁) 苯· 經满部中央標準局員工消費合作社印掣 表I ΈΜ 早層 BaTiO, 介電常數 伸長率 剝離強废 號碼 薄膜* iwt.%、 (%) (ml 1C KJ 0 3.8 48.9 13 1 KJ 15 4.7 32.2 12.8 2 KJ 30 9.8 19.2 12.6 3 KJ 40 11.7 12.6 12.3 -16- 本紙張尺廣读用中固_____ ____ 平 个 ί r ,1 一 - 发 % 9 2 528775 A7 B7 五、發明説明（ 14 4 KJ 50 15.2 8.4 10.6 5 KJ 56 17.3 4.7 9.8 6 KJ 63 26.6 3.0 8.7 7 KJ 73 32.0 2.5 7.2 8 LJ 50 9.6 5.7 6.8 9 LJ 60 12.3 4.5 6.5 *KJ : Kapton® KJ 係 —種熱塑性共聚醯亞胺薄膜， 由70至
*LJ 95莫耳％4,4、氧苯二酸二酐，5至3〇莫耳％苯均四 酸二酐及100莫耳。/。丨，3 ·雙（4 _氨基苯氧基）苯所衍 生，市面上可自杜邦公司購得 Kapton® LJ係一種熱塑性共聚醯亞胺薄膜，由8〇至 95莫耳/〇l，j -雙（4 -氨基苯氧基）苯，5至2〇莫耳％ 六亞甲二胺及100莫耳％4,4，_氧苯二酸二酐所衍 生 (請先閱讀背面之注意事項再填寫本頁) 經满部中央標準局負工消費合作社印製 f例1 0 實例將説明一種高介電常數聚醯亞胺薄膜，其係由7〇 至95莫耳％4,4’-氧苯二酸二酐，5至3〇莫耳％笨均四酸二 酐及100莫耳％1，3_雙（4_氨基苯氧基）苯，含切重量％ PbSn03陶磁填料所衍生之熱塑性共聚酿亞胺薄膜單層所级0 成，具有介電常數約U.3 (1廳，RT)及伸長率爲12、 % 0 . 實例1 1 實例U將説明-種本發明之高介電常數單層聚驢亞胺薄 -17 t紙張尺度剌巾關家標準（CNS ) A4規格（21〇^97^5" 528775 A7 B7 五、發明説明（15 ) 膜，其係由含有7 2重量％陶磁填料混合物一由5 0重量％未 塗覆鈦酸鋇粒子及5 0重量％經7重量％聚醯亞胺塗覆之鈦酸 鋇粒子所形成一之Kapton® K J熱塑性聚醯亞胺所組成。 聚醯亞胺薄膜之機械及電氣性質列示於表11。
表II 機械性質 厚度 伸長率 抗張強度 模量 (mil) (%} (Kpsi) (Kpsi) 機器縱向 2.13 12.3 18.5 620 機器橫向 2.11 11.7 18.8 680 電氣性質 介電 功耗 電容 介電強度 常數 因數 fpfarads/in2) rv/min 在lKHz，RT下測量 33.4 0.004 3360 2500 在lMHz，RT下測量 jjA 0.018 2990 2500 實例1 2 經滴部中央標準局員工消費合竹社印製 (讀先閱讀背面之注意事項再填寫本頁) 實例1 2將説明一種厚度2密爾（Mils)之本發明高介電常 數多層聚醯亞胺薄膜，其係藉將含有5 0重量％鈦酸鋇之中 間1.5密爾厚Kapton® HA聚醯亞胺層與各含45重量％鈦酸 鋇之外0.25密爾厚Kapton® KJ聚醯亞胺黏著性層共擠壓而 製備。 共擠壓多層聚醯亞胺薄膜之機械及電氣性質列示於表 III。 18- 本紙張尺度適用中國國家標準（CNS ) A4規格（210X 297公釐） 528775 A7 B7 五、發明説明（16 )
表III 機械性質 厚度 伸長率 抗張強度 模量 imil) (%) fKpsi) (Kpsi) 機器縱向 1.96 8.7 16.6 658 機器橫向 1.99 5.8 17.1 703 電氣性質 介電 功耗 電容 介電強度 常數 因數 ipfarads/in2) (V/mil) 在lKHz，RT下測量 8.4 0.004 850 2600 在lMHz,RT下測量 8.0 0.015 700 2600 (請先閲讀背面之注意事項再填寫本頁) 斧 ί 丁 "口 實例1 3至2 1 實例1 3至2 1將説明含有單一填料或填料混合物之本發明 高介電常數多層聚醯亞胺薄膜。實例1 3至1 5，1 9及2 0爲2 密爾厚度高介電常數多層聚醯亞胺薄膜，其中間熱固性聚 醯亞胺層具厚度爲1.7密爾，而其外熱塑性黏著性聚醯亞胺 層各具厚度爲0.15密爾，且中間層或中間及外層兩者含有 不同量之欽酸鋇。 經滴部中央標準局員工消費合作社印製 實例1 6至1 8爲類似2密爾厚度多層聚醯亞胺薄膜，其中 間熱固性聚醯亞胺層含有5 0重量％鈦酸鋇與1 5重量％經 Zelec® ECP 3 005XC塗覆之矽氧粒子之混合物，而其外黏 著性熱塑性聚醯亞胺層則含有0至5 0重量％鈦酸鋇。 實例2 1爲1.3密爾厚度多層聚醯亞胺薄膜，其係由0.80密 爾熱固性聚醯亞胺層及0.50密爾黏合於一面且兩層皆含有 _-19- 本紙張尺度適用中國國家標準（CNS ) A4規格（210X297公釐） 528775 A7 B7 五、發明説明（17 ) 鈦酸鋇之熱塑性黏著性聚醯亞胺層所組成。 表IV摘列多層薄膜之介電常數及伸長率。 表IV 實例 多層薄膜* BaTiO, 介電常數 伸長率 號碼 厚度(mil) iWt.%) ilMHz· RT) (%) 13 0.15KJ/1.7HA/0.15KJ 0/50/0 7.6 11.2 14 0.15KJ/1.7HA/0.15KJ 30/50/30 8.9 6.6 15 0.15KJ/1.7HA/0.15KJ 30/63/30 14.3 4.7 ιυ 0.15KJ/1.7HA/0.15KJ 0/50+15Z**/0 8.5 11.7 17 0.15KJ/1.7HA/0.15KJ 30/50+15Z**/30 12.4 9.8 18 0.15KJ/1.7HA/0.15KJ 50/50+15Z**/50 13.8 7.6 19 0.15KJ/1.7HA/0.15KJ 40/50/40 11.1 5.8 20 0.15KJ/1.7HA/0.15KJ 50/50/50 12.7 5.3 21 0.80HA/0.50KJ 50/30 9.3 9.5 *ΗΑ :Kapton® HA 係一 種聚醯亞胺薄膜，由苯均四酸二 (請先閱讀背面之注意事項再填寫本頁) 及4，4 ’ -二氨基二苯基醚所衍生，市面上可自杜邦公 司購得。 * *Z : Zelec® ECP 3005XC係一種具分子篩結構之經摻雜 經濟部中央標準局員工消費合作社印製 銻之氧化錫塗覆之矽氧殼塡料，市面上可自杜邦公 司購得。 實例2 2至2 7 實例2 2至2 7將説明含有1 5重量％聚醯胺酸一由4，4 ’ -氧 20- 本紙張尺度適用中國國家標準（CNS ) A4規格（210X 297公釐） 528775 A7 __ ----------—-— __ 五、發明説明（18 ) 笨二酸二酐，苯均四酸二酐及1，3 -雙（4 -氨基苯氧基）苯溶 於二甲基乙醯胺所衍生一之液體熱塑性聚醯胺酸之製備， 以液體聚醯胺酸塗覆陶磁鈦酸鋇填料粒子及將經塗覆之鈦 酸鋇粒子熱壓縮模製而成層合於銅箔之高介電常數聚醯亞 胺複合物。 聚醯胺酸係由1，3 -雙（4 -氨基苯氧基）苯（20.0克）於2 0分 鐘内一邊攪拌一邊溶于25毫升外I:淀而製備。將18克苯均四 酸二酐及4克4，4 ·-氧苯二酸二酐之固體混合物，以一次一 克，於總共2小時内加至該溶液中。最後的〇.8〇克固體混合 物部份，係以每1 5至2 0分0.2克之速度緩慢加入。該1 5重 量％聚酷亞胺酸溶液之最後黏度爲自1 〇 〇至2 〇 〇 〇泊。 將不同量之鈦酸鋇粒子分別與156毫升份之吡啶與二曱基 乙醯胺之混合物摻合3分鐘。然後將3 0毫升之吡啶-二甲基 乙醯胺漿體於.1小時内加至1 〇〇克之1 5重量％聚醯胺酸液 體，並一邊攪拌。將丙酮與甲醇之混合物（1〇〇克）加入，並 將混合物攪拌1 〇分鐘。將混合物過濾，用丙酮-甲醇洗滌 固體產物，並於6 0。〇下眞空烘乾（但未完全醯亞胺化）。將 經濟部中央標率局員工消費合作社印製 -------- ' 水------1T (讀先閱讀背面之注意事項再填寫本頁) 所得表面面塗覆聚醯胺酸之鈦酸鋇填料研磨至粒度小於i 〇 微米。 將銅箔層放在具厚度7至125微米之Kapton® Η聚醯亞胺 薄膜隔離物旁邊。將經聚醯胺酸表面塗層之鈦酸鋇填料粒 子放在薄膜隔離物中央。 將複合物放在金屬板中間並自280。(：至420。〇下層合5至4 小時’較佳在350。〇下3 0分鐘，以使聚醯胺酸完全聚醯胺 -------- - 21 - 本紙張尺度 528775 A7 B7 五、發明説明（19 ) 經滴部中央標準局員工消費合作社印製 酸硬化而成聚醯亞胺。 複合物之介電常數及剝離強度列示 於表V。 表V 實例 BaTiO, 介電常數 剝離強度 號碼 ·%) QMHz. RT) ipsi) 22 60 15 12 23 70 25 9 24 80 44 6 25 85 51 5 26 87 ! 78 3 27 92 164 2 實例28至34 實例2 8至3 4將説明本發明高介電常數單層熱塑性或熱固 性聚si亞胺薄膜之製備 ，其法係將實例2 2至2 7製備並含有 達9 1重量。/。鈦酸鋇粒子之聚醯胺酸液體塗覆成薄層並使其 硬化而成最終聚醯亞胺薄膜。結果列示於表V I 〇 表VI 實例 單層 BaTi03 厚度 介電常數 號碼 薄膜* (Weight.%) ^Micrometers) (MHz. RT、 28 HA 80 3.7 63 29 HA 91 3.1 137 30 KJ 78 9.1 65 31 KJ 85 7.3 89 I ' I i n I m I' ^ m im n ϋ— n m (請先閲讀背面之注意事項再填寫本頁) -22- 本紙張尺度適用中國國家標準（CNS ) A4規格（2〗0'乂297公釐） 528775 A7 B7 五、發明説明（20 ) 32 LJ 75 6.8 53 ο η LJ 80 8.0 60 34 JP 87 3.2 96 JP : Kapton® JP 是 一種聚 驢亞胺薄膜， 由5 5莫耳％ 3,3 ’，4,4、聯苯四羧酸二酐，4 5莫耳％苯均四酸二 酐及100莫耳％4,4·-二氨基二苯醚所衍生。 獲得極薄之聚醯亞胺薄膜，其含有高量鈦酸鋇且介電常 數自53至137。 (讀先閱讀背面之注意事項再填寫本頁) 經濟部中央標準局員工消費合竹社印繁 -- 本紙張尺度適用中國國家標準（CNS ) Α4規格（210X297公釐）
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- 528775 第087109894號申請專利案 中文申請專利範圍修正本(91年6月） A B c D /年 ί ^y-1 六、申請專利範圍 1. 一種高介電常數撓性.聚醯亞胺薄膜，包含單層之黏著性熱 塑性聚醯亞胺薄膜，其中以薄膜之重量為準分散有4至85 重量％之鐵電陶磁填料，其中該聚醯亞胺薄膜之介電常數 為自4至60，該陶磁填料額外包括導電皮/芯微粒填料， 其中陶磁填料包含鈦酸鋇，且該黏著性熱塑性聚醯亞胺薄 膜包含共聚醯亞胺，其含有60至9 8莫耳％由4,4^氧苯二酸 二酐及具以下化學式之芳族醚二胺衍生之重複醯亞胺單元 η7·ν 〇-ΝΗ- 及2至40莫耳％具以下化學式之額外重複醯亞胺單元 〇 II 〇 II Μ R N~R' C C. II π 〇〇 其中R為芳族四價基及R1為含有至少二個碳原子之芳族 或脂族二胺之二價基，及二胺之二個氨基各附於二價基 之個別碳原子。 2.根據申請專利範圍第1項之高介電常數撓性聚醯亞胺薄 膜，其中陶磁填料係自以下所組成之族群中所選出： 本纸張尺度適用中國國家標準(CNS) A4規格(210X 297公釐） 528775 ABCD 申請專利範圍 BaTi〇3，SrTi〇3，Mg2Ti〇4，Bi2(Ti〇3)3，PbTi〇3， NiTi〇3 J CaTi〇3 5 ZnTi〇3 > Zn2Ti〇4 , BaSn03 ^ Bi(Sn03)3，CaSn〇3，pbSn〇3，MgSn〇3，SrSn〇3， ZnSn〇3，BaZr〇3，CaZr〇3，PbZn〇3，MgZn03，SrZr〇3 及 ZnZr03 〇 3·根據申請專利範圍第2項之高介電常數撓性聚醯亞胺薄 膜’其中陶磁填料之粒度自〇.10至10微米及介電常數自 100 至 30,〇〇〇 〇 4·根據申請專利範圍第丨項之高介電常數撓性聚醯亞胺薄 膜’其中陶磁填料之存在量為2〇至65重量％，且薄膜之 介電常數為自1〇至27。 5·根據申請專利範圍第丨項之高介電常數撓性聚醯亞胺薄 膜’其中陶磁填料包含陶磁填料之混合物。 6·根據申請專利範圍第丨項之高介電常數撓性聚醯亞胺薄 膜’其中陶磁填料表面塗覆熱塑性或熱固性聚醯亞胺。 7·根據申請專利範圍第6項之高介電常數撓性聚醯亞胺薄 膜’其中經表面塗覆之陶磁填料包含表面以衍生自苯均 四酸二酐及4，4’-二氨基二苯基醚之熱固性聚醯亞胺塗覆 之欽fee鎖。 8·根據申凊專利範圍第6項之高介電常數撓性聚醯亞胺薄 膜，其中經表面塗覆之陶磁填料包含表面以衍生自4,4,_ 氧苯二酸二酐，苯均四酸二酐及、、雙”·氨基苯氧基） 苯之熱塑性聚醯亞胺塗覆之鈦酸鋇。 9·根據申請專利範圍第6項之高介電常數撓性聚醯亞胺薄 -2 - 528775 A8 、申請專利範圍 膜’其中經表面塗覆之陶磁填料包含表面以衍生自 ，4,4··聯苯四幾酸二纤，苯均四酸二奸及a〆，·二氨 基二苯基瞇之熱固性聚醯亞胺塗覆之鈦酸鋇。 10·根據申請專利範圍第1項之高介電常數撓性聚醯亞胺薄 膜，其中黏著性熱塑性聚醯亞胺薄膜係包含7〇至95莫耳 竓4,4 -氧豕一酸二肝，5至30莫耳％苯均四酸二肝及1〇〇 莫耳％1，3-雙（4-氨基苯氧基）苯之共聚物。 裝 11·根據申請專利範圍第i項之高介電常數撓性聚醯亞胺薄 膜，其中黏著性熱塑性聚醯亞胺薄膜係包含8 〇至9 5莫耳 、％1，3·雙（4-氨基苯氧基）苯，5至2〇莫耳％六亞甲二胺及 丄❽❹莫耳％々〆1-氧苯二酸二酐之共聚物。 線 12· —種高介電常數撓性多層聚醯亞胺薄膜，包含中間熱塑 性或熱固性聚醯亞胺薄膜層，其一面或二面具黏著性熱 塑性聚醯亞胺薄膜層且至少一層聚醯亞胺層中分散以薄 膜重量為準4至85重量％之鐵電陶磁填料，其中該多層聚 酿亞胺薄膜之介電常數為自4至60，該陶磁填料額外包 括導電皮/芯微粒填料，其中陶磁填料包含鈦酸鋇，且 該黏著性熱塑性聚醯亞胺薄膜包含共聚醯亞胺，其含有 60至98莫耳％由4,4’ -氧苯二酸二纤及具以下化學式之芳 族醚二胺衍生之重複醯亞胺單元-3- 528775 8 8 8 8 ABCD 申請專利範圍 及2至4 0莫耳％具以下化學式之額外重複醯亞胺單元 〇〇 II II /c、八 Nv R N-R C C μ丨4 〇 〇 其中R為芳族四價基及R1為含有至少二個碳原子之芳族 或脂族一胺之二價基，及二胺之二個氨基各附於二價基 之個別碳原子。 13·根據申請專利範圍第1 2項之高介電常數撓性多層聚醯亞 胺薄膜，其中陶磁填料係自以下所組成之族群中所選 出：BaTi〇3 , SrTi03，Mg2Ti04，Bi2(Ti03)3，PbTi03， NiTi03，CaTi03，ZnTi03，Zn2Ti04，BaSn03， Bi(Sn03)3，CaSn03，PbSn03，MgSn03，SrSn03， ZnSn03，BaZr03，CaZr03，PbZn03，MgZn03，SrZrO: 及:^nZr03 o 14· 請專利範圍第12項之高介電常數撓性多層聚醯亞 中陶磁填料包含陶磁填料之混合物。 ..Ά'丨 15·板.争請專利範圍第1 2項之高介電常數撓性聚酿亞胺薄 膜，其中陶磁填料表面塗覆熱塑性或熱固性聚醯亞胺。 16·根據申請專利範圍第1 5項之高介電常數撓性聚醯亞胺薄 膜，其中經表面塗覆之陶磁填料包含表面以衍生自苯均 4 本纸張尺度適用中國國家標準(CNS) A4規格(210X297公釐) 528775 ABCD 六、申請專利範圍 四酸二Sf及4，4，-二氨基二苯基醚之熱固性聚醯亞胺塗覆 之鈥酸鋇。 17·根據申請專利範圍第丨5項之高介電常數撓性聚醯亞胺薄 膜，其中經表面塗覆之陶磁填料包含表面以衍生自4,4，_ 氧苯二酸二酐，苯均四酸二酐及^弘雙。-氨基苯氧基） 苯之熱塑性聚醯亞胺塗覆之鈦酸鋇。 18. 根據申請專利範圍第丨5項之高介電常數撓性聚醯亞胺薄 膜’其中經表面塗覆之陶磁填料包含表面以衍生自 3,3、4,4’-聯苯四羧酸二酐，苯均四酸二酐及4,4、二氣 基二苯基趟之熱固性聚醯亞胺塗覆之鈦酸鋇。 19. 根據申請專利範圍第丨2項之高介電常數撓性多層聚醯亞 胺薄膜’其中陶磁填料包含表面塗覆聚醯亞胺之陶磁填 料與未塗覆填料之混合物。 20·根據申請專利範圍第丨9項之高介電常數撓性多層聚醯亞 胺薄膜’其中陶磁填料包含經聚醯亞胺塗覆之鈇酸鋇與 未塗覆之鈦酸鋇之混合物。 21·根據申請專利範圍第丨2項之高介電常數撓性多層聚醯亞 胺薄膜’其中中間聚醯亞胺薄膜層含有4〇至75重量％之 陶磁填料’而黏著性熱塑性聚醯亞胺薄膜層則含有2 0至 5 0重量％之陶磁填料。 22·根據申請專利範圍第12項之高介電常數撓性多層聚醯亞 胺薄膜，其中中間聚醯亞胺薄膜層之厚度自5至12〇微 米，而黏著性熱塑性薄膜層之厚度則自5至60微米。 23.根據申請專利範圍第12項之高介電常數撓性多層聚醯亞528775 A8胺薄膜’包含自苯均四酸二酐與4,4，-二氨基二苯基醚衍 生之中間熱固性聚醯亞胺層，及自4,4，_苯二酸二酐，苯 均四酸一奸及1，3_雙（4_氨基苯氧基）苯衍生之外部熱塑 性黏著性聚醯亞胺層。 裝 24· —種高介電常數聚醯亞胺液體，包含溶于丨❹至％重量％ •if性有機溶劑中之！至30重量％熱塑性或熱固性聚醯胺 酸，其中分散4至90重量％之鐵電陶磁填料且其介電常數 為4至300，其中該陶磁填料辱外包括導電皮/芯微粒填 料，其中陶磁填料包含鈦酸鋇，且該黏著性熱塑性聚醯 亞胺薄膜包含共聚醯亞胺，其含有6〇至98莫耳％由4,4、 氧苯二酸二酐及具以下化學式之芳族醚二胺衍生之重複 醯亞胺單元 ΓNJH， 訂 線 及2至40莫耳％具以下化學式之額外重複醯亞胺單元 〇 〇 η II /C、 /C、 N、，R、 c c . II Π Ο Ο -6 - 528775 A8 C8 D8 、申請專利範圍 其中R為芳族四價基及R1為含有至少二個碳原子之芳族 或脂族二胺之二價基，及二胺之二個氨基各附於二價基 之個別碳原子。 25. 根據申請專利範圍第24項之高介電常數聚醯亞胺液體， 其中陶磁填料係自以下所組成之族群中選出：BaTi03， SrTi03，Mg2Ti04，Bi2(Ti03)3，PbTi03，NiTi03， CaTi03，ZnTi03，Zn2Ti04，BaSn03，Bi(Sn03)3， CaSn03 ，PbSn03 ，MgSn03 ，SrSn03 ，ZnSn03 ， BaZr03，CaZr03，PbZn03，MgZn03，SrZr03 及 ZnZr〇3 0 26. 根據申請專利範圍第24項之高介電常數聚醯亞胺液體， 其中陶磁填料表面塗覆熱塑性或熱固性聚醯胺。 27. 根據申請專利範圍第24項之高介電常數聚醯亞胺液體， 其中陶磁填料包含經聚醯亞胺塗覆表面之陶磁填料與未 塗覆之陶磁填料之混合物。 28. —種高介電常數撓性聚醯亞胺薄膜，包含單層熱固性聚 醯亞胺，其中以薄膜之重量為準分散4至85重量％之表面 經熱塑性或熱固性聚醯亞胺塗覆之陶磁填料，其中該聚 醯亞胺薄膜之介電常數為4至60，該陶磁填料額外包括 導電皮/芯微粒填料，其中陶磁填料包含鈦酸鋇，且該 黏著性熱塑性聚醯亞胺薄膜包含共聚醯亞胺，其含有60 至98莫耳％由4，4·-氧苯二酸二酐及具以下化學式之芳族 醚二胺衍生之重複醯亞胺單元 本紙張尺度適用中國國家標準(CNS) A4規格(210X 297公釐） 裝 玎 線 528775 A8 一 B8 C8及2至40莫耳％具以下化學式之額外重複醯亞胺單元 〇 〇 II II N R N-R N ^ N / C C . II li 〇 〇 八中11為^•族四價基及R為含有至少二個碳原子之芳族 或脂族二胺之二價基，及二胺之二個氨基各附於二價基 之個別碳原子。 29. 根據申請專利範圍第2 8項之高介電常數撓性聚醯亞胺薄 膜，其中經表面塗覆之陶磁填料包含表面以衍生自苯均 四酸二酐及4,4，_二氨基二苯基醚之熱固性聚醯亞胺塗覆 之鈦酸鋇。 30. 根據申請專利範圍第28項之高介電常數撓性聚醯亞胺薄 膜，其中經表面塗覆之陶磁填料包含表面以衍生自4,4,_ 氧苯二酸二酐，苯均四酸二酐及1，3_雙（4氨基苯氧基） 苯之熱塑性聚醯亞胺塗覆之鈦酸鋇。 31. 根據申請專利範圍第28項之高介電常數撓性聚醯亞胺薄 -8-528775 A8 B8 C8 D8膜，其中經表面塗覆之陶磁填料包含以衍生自3,3，，4,4,_ 聯苯四羧酸二酐及4,4，-二氨基二苯基醚之熱固性聚醯亞 胺塗覆之鈦酸鋇。 32.根據申請專利範圍第2 8項之高介電常數撓性聚醯亞胺薄 膜，其中經表面塗覆之陶磁填料包含經熱塑性或熱固性 聚醯亞胺塗覆之陶磁填料及未塗覆之陶磁填料。 33· —種製備高介電常數聚醯亞胺複合物之方法，包含將表 面經聚醯亞胺塗覆之陶磁填料於溫度28〇 t至42〇充下壓 縮模製或溶體擠壓5至4小時，其中複合物之介電常數為 1 5至170，該陶磁填料額外包括導電皮/芯微粒填料， 其中陶磁填料包含鈦酸鋇，且該黏著性熱塑性聚醯亞胺 薄膜包含共聚醯亞胺，其含有60至98莫耳％由4,4，-氧苯 二酸二酐及具以下化學式之芳族醚二胺衍生之重複醯亞 胺單元及2至40莫耳％具以下化學式之額外重複醯亞胺單元 〇〇 II II 八八 n、，R、严R. C C -9- 本紙張尺度適用中國國家標準(CNS) A4規格(210X297公爱) A8 528775 BCD 々、申請專利範圍 其中R為芳族四價基及R1為含有至少二個碳原子之芳族 或脂族二胺之二價基，及二胺之二個氨基各附於二價基 之個別碳原子。 34. 根據申請專利範圍第3 3項之方法，其中表面經聚醯亞胺 塗覆之陶磁填料包含表面以衍生自4,4、氧苯二酸二酐， 苯均四酸二酐及1，3-雙（4-氨基苯氧基）苯之熱塑性聚醯 亞胺塗覆之鈦酸鋇。 35. —種高介電常數聚醯亞胺複金物，其係根據申請專利範 圍第33項之方法製備並層合於銅箔層。 ^紙張尺度適用中國國家標準(CNS) A4規格(210X297公釐）
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- 1998-04-09 EP EP19980302799 patent/EP0902048B1/en not_active Expired - Lifetime
- 1998-04-10 KR KR1019980012750A patent/KR100284461B1/ko not_active IP Right Cessation
- 1998-04-10 JP JP9963098A patent/JP3133976B2/ja not_active Expired - Fee Related
- 1998-06-19 TW TW87109894A patent/TW528775B/zh not_active IP Right Cessation
- 1998-12-29 US US09/222,103 patent/US6159611A/en not_active Expired - Lifetime
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN111393806A (zh) * | 2020-03-10 | 2020-07-10 | 深圳市信维通信股份有限公司 | 液晶聚酯薄膜及其制备方法 |
| CN111393806B (zh) * | 2020-03-10 | 2023-03-17 | 深圳市信维通信股份有限公司 | 液晶聚酯薄膜及其制备方法 |
Also Published As
| Publication number | Publication date |
|---|---|
| JP3133976B2 (ja) | 2001-02-13 |
| US6150456A (en) | 2000-11-21 |
| DE69832444D1 (de) | 2005-12-29 |
| EP0902048A1 (en) | 1999-03-17 |
| EP0902048B1 (en) | 2005-11-23 |
| JPH11106650A (ja) | 1999-04-20 |
| KR19990029156A (ko) | 1999-04-26 |
| US6159611A (en) | 2000-12-12 |
| DE69832444T2 (de) | 2006-08-03 |
| KR100284461B1 (ko) | 2001-03-02 |
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