CN109843994A - 片状预浸料 - Google Patents
片状预浸料 Download PDFInfo
- Publication number
- CN109843994A CN109843994A CN201780063794.8A CN201780063794A CN109843994A CN 109843994 A CN109843994 A CN 109843994A CN 201780063794 A CN201780063794 A CN 201780063794A CN 109843994 A CN109843994 A CN 109843994A
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- Prior art keywords
- compound
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- weight
- solidification compound
- solidification
- Prior art date
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- 150000001875 compounds Chemical class 0.000 claims abstract description 162
- 238000007711 solidification Methods 0.000 claims abstract description 91
- 230000008023 solidification Effects 0.000 claims abstract description 91
- 239000000463 material Substances 0.000 claims abstract description 68
- 239000003795 chemical substances by application Substances 0.000 claims abstract description 58
- 150000002118 epoxides Chemical class 0.000 claims abstract description 46
- 239000003054 catalyst Substances 0.000 claims abstract description 18
- 230000009477 glass transition Effects 0.000 claims abstract description 16
- 239000000203 mixture Substances 0.000 claims abstract description 12
- 239000000945 filler Substances 0.000 claims description 23
- 239000000758 substrate Substances 0.000 claims description 15
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 12
- 125000000524 functional group Chemical group 0.000 claims description 12
- 239000003566 sealing material Substances 0.000 claims description 12
- 238000004806 packaging method and process Methods 0.000 claims description 6
- 239000007787 solid Substances 0.000 claims description 6
- 238000000748 compression moulding Methods 0.000 claims description 5
- MTHSVFCYNBDYFN-UHFFFAOYSA-N diethylene glycol Chemical compound OCCOCCO MTHSVFCYNBDYFN-UHFFFAOYSA-N 0.000 description 102
- 238000001723 curing Methods 0.000 description 65
- -1 bis- (methylol)-n-butyl alcohols Chemical class 0.000 description 42
- 238000004519 manufacturing process Methods 0.000 description 30
- 229920000647 polyepoxide Polymers 0.000 description 29
- 239000004593 Epoxy Substances 0.000 description 28
- 239000000126 substance Substances 0.000 description 28
- GYZLOYUZLJXAJU-UHFFFAOYSA-N diglycidyl ether Chemical compound C1OC1COCC1CO1 GYZLOYUZLJXAJU-UHFFFAOYSA-N 0.000 description 27
- 239000003822 epoxy resin Substances 0.000 description 27
- 238000000034 method Methods 0.000 description 23
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 21
- 150000008065 acid anhydrides Chemical class 0.000 description 20
- 238000010438 heat treatment Methods 0.000 description 19
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 17
- 150000001991 dicarboxylic acids Chemical class 0.000 description 16
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- PEDCQBHIVMGVHV-UHFFFAOYSA-N Glycerine Chemical compound OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 description 12
- 125000003118 aryl group Chemical group 0.000 description 12
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- 239000011347 resin Substances 0.000 description 12
- 229910052799 carbon Inorganic materials 0.000 description 11
- 239000004065 semiconductor Substances 0.000 description 11
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 10
- 239000004745 nonwoven fabric Substances 0.000 description 10
- 238000002360 preparation method Methods 0.000 description 10
- 150000008064 anhydrides Chemical class 0.000 description 9
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- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 9
- 229910052710 silicon Inorganic materials 0.000 description 9
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- 125000002723 alicyclic group Chemical group 0.000 description 8
- 125000001931 aliphatic group Chemical group 0.000 description 8
- IISBACLAFKSPIT-UHFFFAOYSA-N bisphenol A Chemical compound C=1C=C(O)C=CC=1C(C)(C)C1=CC=C(O)C=C1 IISBACLAFKSPIT-UHFFFAOYSA-N 0.000 description 8
- 230000000694 effects Effects 0.000 description 8
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 8
- RIOQSEWOXXDEQQ-UHFFFAOYSA-N triphenylphosphine Chemical compound C1=CC=CC=C1P(C=1C=CC=CC=1)C1=CC=CC=C1 RIOQSEWOXXDEQQ-UHFFFAOYSA-N 0.000 description 8
- ZWEHNKRNPOVVGH-UHFFFAOYSA-N 2-Butanone Chemical compound CCC(C)=O ZWEHNKRNPOVVGH-UHFFFAOYSA-N 0.000 description 7
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- 150000002148 esters Chemical group 0.000 description 7
- 239000000123 paper Substances 0.000 description 7
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- 238000007789 sealing Methods 0.000 description 7
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- 239000002253 acid Substances 0.000 description 6
- PXKLMJQFEQBVLD-UHFFFAOYSA-N bisphenol F Chemical compound C1=CC(O)=CC=C1CC1=CC=C(O)C=C1 PXKLMJQFEQBVLD-UHFFFAOYSA-N 0.000 description 6
- 239000011951 cationic catalyst Substances 0.000 description 6
- 125000000113 cyclohexyl group Chemical group [H]C1([H])C([H])([H])C([H])([H])C([H])(*)C([H])([H])C1([H])[H] 0.000 description 6
- 239000001301 oxygen Substances 0.000 description 6
- 229910052760 oxygen Inorganic materials 0.000 description 6
- VPWNQTHUCYMVMZ-UHFFFAOYSA-N 4,4'-sulfonyldiphenol Chemical class C1=CC(O)=CC=C1S(=O)(=O)C1=CC=C(O)C=C1 VPWNQTHUCYMVMZ-UHFFFAOYSA-N 0.000 description 5
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 5
- 229930185605 Bisphenol Natural products 0.000 description 5
- 239000004215 Carbon black (E152) Substances 0.000 description 5
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical class OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 5
- DNIAPMSPPWPWGF-UHFFFAOYSA-N Propylene glycol Chemical compound CC(O)CO DNIAPMSPPWPWGF-UHFFFAOYSA-N 0.000 description 5
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- FVCSARBUZVPSQF-UHFFFAOYSA-N 5-(2,4-dioxooxolan-3-yl)-7-methyl-3a,4,5,7a-tetrahydro-2-benzofuran-1,3-dione Chemical compound C1C(C(OC2=O)=O)C2C(C)=CC1C1C(=O)COC1=O FVCSARBUZVPSQF-UHFFFAOYSA-N 0.000 description 4
- CTKINSOISVBQLD-UHFFFAOYSA-N Glycidol Chemical compound OCC1CO1 CTKINSOISVBQLD-UHFFFAOYSA-N 0.000 description 4
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- KKEYFWRCBNTPAC-UHFFFAOYSA-N Terephthalic acid Chemical compound OC(=O)C1=CC=C(C(O)=O)C=C1 KKEYFWRCBNTPAC-UHFFFAOYSA-N 0.000 description 4
- WNLRTRBMVRJNCN-UHFFFAOYSA-N adipic acid Chemical compound OC(=O)CCCCC(O)=O WNLRTRBMVRJNCN-UHFFFAOYSA-N 0.000 description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 4
- WERYXYBDKMZEQL-UHFFFAOYSA-N butane-1,4-diol Chemical compound OCCCCO WERYXYBDKMZEQL-UHFFFAOYSA-N 0.000 description 4
- 230000008859 change Effects 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 4
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- 150000002430 hydrocarbons Chemical class 0.000 description 4
- 150000002989 phenols Chemical class 0.000 description 4
- 229920000768 polyamine Polymers 0.000 description 4
- 230000009467 reduction Effects 0.000 description 4
- 150000003839 salts Chemical class 0.000 description 4
- 239000002904 solvent Substances 0.000 description 4
- 150000005846 sugar alcohols Polymers 0.000 description 4
- KNDQHSIWLOJIGP-UMRXKNAASA-N (3ar,4s,7r,7as)-rel-3a,4,7,7a-tetrahydro-4,7-methanoisobenzofuran-1,3-dione Chemical compound O=C1OC(=O)[C@@H]2[C@H]1[C@]1([H])C=C[C@@]2([H])C1 KNDQHSIWLOJIGP-UMRXKNAASA-N 0.000 description 3
- QTWJRLJHJPIABL-UHFFFAOYSA-N 2-methylphenol;3-methylphenol;4-methylphenol Chemical compound CC1=CC=C(O)C=C1.CC1=CC=CC(O)=C1.CC1=CC=CC=C1O QTWJRLJHJPIABL-UHFFFAOYSA-N 0.000 description 3
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 3
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- LRHPLDYGYMQRHN-UHFFFAOYSA-N N-Butanol Chemical compound CCCCO LRHPLDYGYMQRHN-UHFFFAOYSA-N 0.000 description 3
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 description 3
- 239000002202 Polyethylene glycol Substances 0.000 description 3
- OFOBLEOULBTSOW-UHFFFAOYSA-N Propanedioic acid Natural products OC(=O)CC(O)=O OFOBLEOULBTSOW-UHFFFAOYSA-N 0.000 description 3
- 239000002390 adhesive tape Substances 0.000 description 3
- 150000001298 alcohols Chemical class 0.000 description 3
- 239000004305 biphenyl Substances 0.000 description 3
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 description 3
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- 229930003836 cresol Natural products 0.000 description 3
- 238000005538 encapsulation Methods 0.000 description 3
- 125000003700 epoxy group Chemical group 0.000 description 3
- 239000004744 fabric Substances 0.000 description 3
- 125000004836 hexamethylene group Chemical group [H]C([H])([*:2])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[*:1] 0.000 description 3
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 3
- 238000005470 impregnation Methods 0.000 description 3
- 239000004615 ingredient Substances 0.000 description 3
- NLYAJNPCOHFWQQ-UHFFFAOYSA-N kaolin Chemical compound O.O.O=[Al]O[Si](=O)O[Si](=O)O[Al]=O NLYAJNPCOHFWQQ-UHFFFAOYSA-N 0.000 description 3
- 238000005259 measurement Methods 0.000 description 3
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 3
- VYKXQOYUCMREIS-UHFFFAOYSA-N methylhexahydrophthalic anhydride Chemical compound C1CCCC2C(=O)OC(=O)C21C VYKXQOYUCMREIS-UHFFFAOYSA-N 0.000 description 3
- 238000002156 mixing Methods 0.000 description 3
- 229920001223 polyethylene glycol Polymers 0.000 description 3
- 235000013824 polyphenols Nutrition 0.000 description 3
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- 239000001294 propane Substances 0.000 description 3
- 239000000377 silicon dioxide Substances 0.000 description 3
- MUTGBJKUEZFXGO-OLQVQODUSA-N (3as,7ar)-3a,4,5,6,7,7a-hexahydro-2-benzofuran-1,3-dione Chemical compound C1CCC[C@@H]2C(=O)OC(=O)[C@@H]21 MUTGBJKUEZFXGO-OLQVQODUSA-N 0.000 description 2
- DNIAPMSPPWPWGF-GSVOUGTGSA-N (R)-(-)-Propylene glycol Chemical compound C[C@@H](O)CO DNIAPMSPPWPWGF-GSVOUGTGSA-N 0.000 description 2
- VILCJCGEZXAXTO-UHFFFAOYSA-N 2,2,2-tetramine Chemical compound NCCNCCNCCN VILCJCGEZXAXTO-UHFFFAOYSA-N 0.000 description 2
- WVRNUXJQQFPNMN-VAWYXSNFSA-N 3-[(e)-dodec-1-enyl]oxolane-2,5-dione Chemical compound CCCCCCCCCC\C=C\C1CC(=O)OC1=O WVRNUXJQQFPNMN-VAWYXSNFSA-N 0.000 description 2
- FKBMTBAXDISZGN-UHFFFAOYSA-N 5-methyl-3a,4,5,6,7,7a-hexahydro-2-benzofuran-1,3-dione Chemical compound C1C(C)CCC2C(=O)OC(=O)C12 FKBMTBAXDISZGN-UHFFFAOYSA-N 0.000 description 2
- ULKLGIFJWFIQFF-UHFFFAOYSA-N 5K8XI641G3 Chemical compound CCC1=NC=C(C)N1 ULKLGIFJWFIQFF-UHFFFAOYSA-N 0.000 description 2
- 239000005995 Aluminium silicate Substances 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- FERIUCNNQQJTOY-UHFFFAOYSA-N Butyric acid Chemical compound CCCC(O)=O FERIUCNNQQJTOY-UHFFFAOYSA-N 0.000 description 2
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 description 2
- 241000551547 Dione <red algae> Species 0.000 description 2
- 241000196324 Embryophyta Species 0.000 description 2
- 239000004386 Erythritol Substances 0.000 description 2
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- 239000004113 Sepiolite Substances 0.000 description 2
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- WDJHALXBUFZDSR-UHFFFAOYSA-M acetoacetate Chemical compound CC(=O)CC([O-])=O WDJHALXBUFZDSR-UHFFFAOYSA-M 0.000 description 2
- 239000001361 adipic acid Substances 0.000 description 2
- 235000011037 adipic acid Nutrition 0.000 description 2
- 239000004411 aluminium Substances 0.000 description 2
- 229910052782 aluminium Inorganic materials 0.000 description 2
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- 235000012211 aluminium silicate Nutrition 0.000 description 2
- ADCOVFLJGNWWNZ-UHFFFAOYSA-N antimony trioxide Chemical compound O=[Sb]O[Sb]=O ADCOVFLJGNWWNZ-UHFFFAOYSA-N 0.000 description 2
- TZCXTZWJZNENPQ-UHFFFAOYSA-L barium sulfate Chemical compound [Ba+2].[O-]S([O-])(=O)=O TZCXTZWJZNENPQ-UHFFFAOYSA-L 0.000 description 2
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- 150000001732 carboxylic acid derivatives Chemical class 0.000 description 2
- YCIMNLLNPGFGHC-UHFFFAOYSA-N catechol Chemical compound OC1=CC=CC=C1O YCIMNLLNPGFGHC-UHFFFAOYSA-N 0.000 description 2
- 150000001768 cations Chemical class 0.000 description 2
- 239000002738 chelating agent Substances 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 238000006482 condensation reaction Methods 0.000 description 2
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- 125000004122 cyclic group Chemical group 0.000 description 2
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- 239000003085 diluting agent Substances 0.000 description 2
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- XBDQKXXYIPTUBI-UHFFFAOYSA-N dimethylselenoniopropionate Natural products CCC(O)=O XBDQKXXYIPTUBI-UHFFFAOYSA-N 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
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- 125000001495 ethyl group Chemical group [H]C([H])([H])C([H])([H])* 0.000 description 2
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- VLKZOEOYAKHREP-UHFFFAOYSA-N methyl pentane Natural products CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 description 2
- 125000000740 n-pentyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 description 2
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- CXMXRPHRNRROMY-UHFFFAOYSA-N sebacic acid Chemical compound OC(=O)CCCCCCCCC(O)=O CXMXRPHRNRROMY-UHFFFAOYSA-N 0.000 description 2
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- 229950004288 tosilate Drugs 0.000 description 2
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- DQVXWCCLFKMJTQ-UHFFFAOYSA-N (4-methylphenoxy)boronic acid Chemical compound CC1=CC=C(OB(O)O)C=C1 DQVXWCCLFKMJTQ-UHFFFAOYSA-N 0.000 description 1
- XGINAUQXFXVBND-UHFFFAOYSA-N 1,2,6,7,8,8a-hexahydropyrrolo[1,2-a]pyrimidine Chemical compound N1CC=CN2CCCC21 XGINAUQXFXVBND-UHFFFAOYSA-N 0.000 description 1
- IVSZLXZYQVIEFR-UHFFFAOYSA-N 1,3-Dimethylbenzene Natural products CC1=CC=CC(C)=C1 IVSZLXZYQVIEFR-UHFFFAOYSA-N 0.000 description 1
- WZCQRUWWHSTZEM-UHFFFAOYSA-N 1,3-phenylenediamine Chemical compound NC1=CC=CC(N)=C1 WZCQRUWWHSTZEM-UHFFFAOYSA-N 0.000 description 1
- PXGZQGDTEZPERC-UHFFFAOYSA-N 1,4-cyclohexanedicarboxylic acid Chemical compound OC(=O)C1CCC(C(O)=O)CC1 PXGZQGDTEZPERC-UHFFFAOYSA-N 0.000 description 1
- DCTOHCCUXLBQMS-UHFFFAOYSA-N 1-undecene Chemical compound CCCCCCCCCC=C DCTOHCCUXLBQMS-UHFFFAOYSA-N 0.000 description 1
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Abstract
本发明提供一种兼具低热线性膨胀系数和高柔软性适当的柔软性,且优抗翘曲性及抗破裂性优异片状预浸料。本发明的片状预浸料,其具有包含热线性膨胀系数为10ppm/K以下的材料的片状多孔性支持体的孔内填充有下述固化性组合物的结构,该片状预浸料的固化物的玻璃化转变温度为‑60℃以上且100℃以下;固化性组合物:是包含固化性化合物(A)、固化剂(B)和/或固化催化剂(C)的组合物,其中,(A)总量的50重量%以上为环氧当量140~3000g/eq的环氧化合物。
Description
技术领域
本发明涉及一种能够用作扇出型晶圆级封装(FOWLP:Fan Out Wafer LevelPackage)用密封材料和基板的抗翘曲材料的片状预浸料。本申请案基于2016年10月17日在日本提出申请的日本特愿2016-203799号而主张优先权,并引用其内容。
背景技术
作为半导体封装的新颖技术/制造方法的扇出型晶圆级封装(FOWLP:Fan OutWafer Level Package)通过将已单片化的半导体芯片再配置在基板上且密封,而制造再构筑晶圆,然后,制造再布线层/BGA等且进行单片化封装的制造方法。
作为上述密封方法,使用了环氧树脂的树脂密封为主流。但是,就树脂密封而言,由于树脂的固化收缩和热膨胀在封装后产生翘曲的问题。这是因为密封树脂的热线性膨胀系数比芯片的热线性膨胀系数大而引起的。
作为降低密封树脂的热线性膨胀系数而防止翘曲的方法,已知有将大量的填料添加到密封树脂中的方法(专利文献1)。但是,添加大量的填料时,密封树脂的熔融粘度会显著地上升,存在使用性降低的问题。而且,由于密封树脂的柔软性降低而变得硬且脆,存在容易产生破裂的问题。
先行技术文献
专利文献
专利文献1:日本特开2004-56141号公报
发明内容
本发明所解决的技术问题
因此,本发明的目的在于提供一种兼具低热线性膨胀系数和高柔软性,抗翘曲性及抗裂性均优异的片状预浸料。
解决本发明技术问题的技术手段
本发明的发明人为解决上述技术问题而进行深入研究,结果发现,包含热线性膨胀系数低的材料的片状多孔支持体,填充含有环氧当量140~3000g/eq的环氧化合物的固化性组合物而得到片状预浸料的固化物,由于热引起的收缩率和膨胀率小,且具有适度的柔软性,因此,所述固化物的抗翘曲性及抗裂性优异。本发明是鉴于上述情况而完成的发明。
即,本发明提供一种片状预浸料,其具有包含热线性膨胀系数为10ppm/K以下的材料的片状多孔性支持体的孔内填充有下述固化性组合物而成的结构,该片状预浸料的固化物的玻璃化转变温度为-60℃以上且100℃以下;
固化性组合物是:包含固化性化合物(A)、固化剂(B)和/或固化催化剂(C)的组合物,其中,(A)总量的50重量%以上为环氧当量140~3000g/eq的环氧化合物。
本发明提供所述片状预浸料,其中,固化性组合物含有固化剂(B),并且使固化剂(B)的比例如下:
相对于固化性化合物(A)的固化性基团1摩尔,固化剂(B)的反应性基团为0.8~1.2摩尔。
本发明提供所述片状预浸料,其中,固化性组合物含有固化性化合物(A)及固化催化剂(C),并且相对于上述(A)100重量份,(C)为0.1~10重量份的比例。
本发明提供所述的片状预浸料,其中,固化性组合物包含的全部固化性化合物(A)(含有固化剂(B)时,为全部固化性化合物(A)与全部固化剂(B))的相对于单个官能团的分子量的加权平均值为180~1000g/eq。
本发明提供所述的片状预浸料,其中,固化性组合物的固化物的热线性膨胀系数为100ppm/K以上,且片状预浸料的固化物的热线性膨胀系数为55ppm/K以下。
本发明提供所述的片状预浸料,其中,固化性组合物含有相对于固化性化合物(A)100重量份为1~50重量份的填料(D)。
本发明提供所述的片状预浸料,其中,片状多孔性支持体的厚度为5~500μm。
本发明提供所述的片状预浸料,其是压缩成形用密封材料。
本发明提供所述的片状预浸料,其是扇出型晶圆级封装用密封材料。
本发明提供所述的片状预浸料,其是厚度100μm以下的薄化硅芯片或薄化基板的抗翘曲材料。
发明的效果
本发明的片状预浸料,可以通过热固化,形成具有适度柔软性、由热引起的收缩率和膨胀率低、且发挥可以表现出优异的抗翘曲性及抗裂性的固化物。因此,本发明的片状预浸料优选用作FOWLP用密封材料及基板的抗翘曲材料。
附图说明
图1表示使用本发明的片状预浸料的FOWLP的制造方法的一个例子的示意图。
图2表示翘曲量的测定方法的图。
具体实施方式
[片状预浸料]
本发明的片状预浸料具有包含热线性膨胀系数为10ppm/K以下的材料的片状多孔性支持体的孔内填充有下述固化性组合物的结构,该片状预浸料的固化物的玻璃化转变温度为-60℃以上且100℃以下。
固化性组合物:是含有固化性化合物(A)、固化剂(B)和/或固化催化剂(C)的组合物,其中,(A)总量的50重量%以上为环氧当量140~3000g/eq的环氧化合物。
[片状多孔性支持体]
本发明的片状多孔性支持体(下文,有时简称为“多孔性支持体”),包含热线性膨胀系数[例如在-20℃~300℃(优选为-10~300℃,特别优选为0~300℃,最优选为0~250℃)的热线性膨胀系数]为10ppm/K以下(优选为7ppm/K以下,特别优选为5ppm/K以下)的材料。本发明的片状预浸料由于使用包含热线性膨胀系数为10ppm/K以下的材料的多孔性支持体,因此能够将固化收缩率及热线性膨胀系数抑制为较小,可以抑制赋予热冲击造成的翘曲,并可以抑制破裂的产生。
作为热线性膨胀系数为10ppm/K以下的材料,例如可举出:纸、纤维素、玻璃纤维、液晶材料等。本发明中,优选纸、纤维素、玻璃纤维,特别是就轻质且容易取得方面,优选纤维素。
多孔性支持体的孔隙率例如90~10vol%,优选为80~30vol%,特别优选为70~30vol%,最优选为70~50vol%。孔隙率低于上述范围时,存在下述倾向:难以含浸充分量的后述固化性组合物,不易得到表面平滑性。另一方面,孔隙率高于上述范围时,存在下述倾向:无法充分地得到通过多孔性支持体得到的增强效果,而且难以将固化收缩率及热线性膨胀系数抑制为较小。
需要说明的是,在本说明书的所谓“孔隙率”表示,在多孔性支持体中的孔隙的体积率。多孔性支持体的孔隙率,可对于10cm×10cm的试样测定其表面面积、厚度及质量,且从下述计算式算出。在此,Ar为多孔性支持体的面积(cm2),t为厚度(cm),W为多孔性支持体的质量(g),M为多孔性支持体的材料的密度。多孔性支持体的厚度(t)使用膜厚计(PEACOK公司制PDN-20),对于多孔性支持体的各种位置进行10点测定且采用其平均值。
孔隙率(vol%)={1-W/(M×Ar×t)}×100
多孔性支持体的厚度,例如5~500μm。下限优选为10μm,特别优选为15μm,最优选为20μm。而且,上限优选为300μm,优选为200μm,特别优选为100μm,最优选为75μm。多孔性支持体的厚度能够在上述范围适当地进行调整,例如当固化性组合物单独的固化物的Tg较低时,可通过将多孔性支持体薄化而将固化收缩率抑制为较小。固化性组合物单独的固化物的Tg提高时,可通过将多孔性支持体增厚而将热线性膨胀系数抑制为较小。多孔性支持体的厚度高于上述范围时,存在难以应对电子机器的小型化、轻质化的要求的倾向。另一方面,厚度低于上述范围时,难以得到充分的强韧性,例如用作FOWLP用密封材料时,会变得难以通过封装而进行高强度化,即使用作抗翘曲剂时,存在难以防止经薄化的硅芯片和基板发生翘曲的倾向。
[固化性组合物]
本发明的固化性组合物是含有固化性化合物(A)、固化剂(B)和/或固化催化剂(C)的组合物,且(A)总量的50重量%以上是环氧当量140~3000g/eq的环氧化合物。
(固化性化合物(A))
固化性化合物(A)中,含有(A)总量的50重量%以上(优选为70重量%以上,特别优选为80重量%以上,最优选为90重量%以上,上限为100重量%)的环氧当量(g/eq)为140~3000(优选170~1000,更优选180~1000,特别优选180~500)的环氧化合物。过量地含有环氧当量脱离上述范围的化合物时,固化性组合物单独的固化物的柔软性降低且抗破裂性降低,故不优选。
环氧化合物包括脂环式环氧化合物、芳香族环氧化合物及脂肪族环氧化合物等。
<脂环式环氧化合物>
作为上述脂环式环氧化合物,包括在分子内具有1个以上的脂环及1个以上的环氧基的公知或惯用的化合物,优选以下的化合物等。
(1)环氧基直接单键键合在脂环上的化合物
(2)在分子内具有脂环及缩水甘油醚基的化合物(缩水甘油醚型环氧化合物)
作为上述(1)的环氧基直接单键键合在脂环的化合物,例如可举出下述式(i)表示的化合物等。
[化学式1]
式(i)中,R≡从p元醇的结构式除去p个羟基(-OH)后的基团(p价有机基团),p、n分别表示自然数。作为p元醇[R≡(OH)p],可举出2,2-双(羟甲基)-1-丁醇等多价醇(碳原子数1~15的醇类等)等。P优选1~6,n优选1~30。p为2以上时,在各个的[]内(外侧的方括号内)的基的n可以相同,也不可以不同。作为上述式(i)表示的化合物,具体而言,可举出2,2-双(羟甲基)-1-丁醇的1,2-环氧基-4-(2-环氧乙烷基)环己烷加成物[例如商品名“EHPE3150”(Daicel株式会社制)等]等。
作为在上述(2)分子内具有脂环及缩水甘油醚基的化合物,例如可举出脂环式醇(特别是脂环式多元醇)的缩水甘油醚。更具体而言,例如可举出:2,2-双[4-(2,3-环氧丙氧基)环己基]丙烷、2,2-双[3,5-二甲基-4-(2,3-环氧丙氧基)环己基]丙烷等双酚A型环氧化合物经氢化而得到的化合物(氢化双酚A型环氧化合物);双[o,o-(2,3-环氧丙氧基)环己基]甲烷、双[o,p-(2,3-环氧丙氧基)环己基]甲烷、双[p,p-(2,3-环氧丙氧基)环己基]甲烷、双[3,5-二甲基-4-(2,3-环氧丙氧基)环己基]甲烷等双酚F型环氧化合物经氢化的化合物(氢化双酚F型环氧化合物);氢化联苯酚型环氧化合物;氢化苯酚酚醛清漆型环氧化合物;氢化甲酚酚醛清漆型环氧化合物;双酚A的氢化甲酚酚醛清漆型环氧化合物;氢化萘型环氧化合物;从三苯酚甲烷得到的环氧化合物经氢化的化合物等。
<芳香族环氧化合物>
作为上述芳香族环氧化合物,例如可举出:通过双酚类[例如双酚A、双酚F、双酚S、芴双酚等]与表卤醇的缩合反应而得到的表双(Epi-Bis)型缩水甘油醚型环氧树脂;通过使该等表双型缩水甘油醚型环氧树脂进一步与上述双酚类进行加成反应而得到的高分子量表双型缩水甘油醚型环氧树脂;后述的改性表双型环氧丙基醚型环氧树脂;通过使酚类[例如苯酚、甲酚、二甲苯酚、间苯二酚、儿茶酚、双酚A、双酚F、双酚S等]与醛[例如甲醛、乙醛、苯甲醛、羟基苯甲醛、水杨醛等]缩合反应而得到的多元醇类,进一步与表卤醇进行缩合反应得到的酚醛清漆-烷基型缩水甘油醚型环氧树脂;在2个苯酚骨架键合于芴环的第9位且从这些苯酚骨架的羟基中除去氢原子的氧原子上,分别直接或经由氧化烯烃基键和有缩水甘油基的环氧化合物等。
作为上述改性表双型缩水甘油醚型环氧树脂,例如可举出下述式(ii)表示的化合物。下述式中,R1~R4可以相同,也可以不同,表示氢原子或烃基。k表示1以上的整数。L1表示低极性键合基团,L2表示柔软性骨架。
[化学式2]
上述烃中包含脂肪族烃基、脂环式烃基、芳香族烃基及它们键合而成的基团。
作为脂肪族烃基,优选碳原子数1~20的脂肪族烃基,例如能够举出:甲基、乙基、丙基、异丙基、丁基、异丁基、仲丁基、叔丁基、戊基、己基、癸基、十二碳基等碳原子数1~20(优选为1~10,特别优选为1~3)左右的烷基;乙烯基、烯丙基、1-丁烯基等碳原子数2~20(优选为2~10,特别优选为2~3)左右的烯基;乙炔基、丙炔基等碳原子数2~20(优选为2~10,特别优选为2~3)左右的炔基等。
作为脂环式烃基,优选以3~10元的脂环式烃基,例如能够举出环丙基、环丁基、环戊基、环己基、环辛基等3~8员(优选为5~8员)左右的环烷基等。
作为芳香族烃基,优选碳原子数6~14(优选为6~10)的芳香族烃基,例如能够举出苯基等。
作为上述R1~R4,其中,优选脂肪族烃基(特别是烷基)。
上述L1表示低极性键合基团,例如能够举出亚甲基、甲基亚甲基、二甲基亚甲基、亚乙基等碳原子数1~3的直链状或支链状亚烷基。
上述L2表示柔软性骨架,例如能够举出碳原子数2~4的氧化烯烃基团。具体而言,可举出氧化乙基、氧化丙烯基、氧化丁烯基、氧四亚甲基等。
由于改性表双型缩水甘油醚型环氧树脂具有上述结构,因此添加在固化性组合物时能够得到提升抗破裂性的效果。
作为上述改性表双型缩水甘油醚型环氧树脂,可适合使用下述式(ii-1)表示的化合物。在本发明,例如可使用商品名“EPICLON EXA-4850-1000”(环氧当量:350,DIC株式会社制造)、商品名“EPICLON EXA-4850-150”(环氧当量:433,DIC株式会社制造)等的市售品。
[化学式3]
<脂肪族环氧化合物>
作为上述脂肪族环氧化合物,例如可举出q价的不具有环状结构的醇(q为自然数)的缩水甘油醚;一元或多元羧酸[例如乙酸、丙酸、丁酸、硬脂酸、己二酸、癸二酸、马来酸、衣康酸等]的缩水甘油酯;环氧化亚麻仁油、环氧化大豆油、环氧化蓖麻油等具有双键的油脂的环氧化物;环氧化聚丁二烯等聚烯烃(包含聚二烯烃)的环氧化物等。需要说明的是,作为上述不具有环状结构的q元醇,例如可举出:甲醇、乙醇、1-丙醇、异丙醇、1-丁醇等一元醇;乙二醇、1,2-丙二醇、1,3-丙二醇、1,4-丁二醇、新戊二醇、1,6-己二醇、二乙二醇、三乙二醇、四乙二醇、二丙二醇、聚乙二醇、聚丙二醇等的二价醇;甘油、二甘油、赤藻糖醇(erythritol)、三羟甲基乙烷、三羟甲基丙烷、季戊四醇、二季戊四醇、山梨糖醇等三元以上的多元醇等。而且,q元醇可为聚醚多元醇、聚酯多元醇、聚碳酸酯多元醇、聚烯烃多元醇等。
(固化剂(B))
构成本发明的固化性组合物的固化剂(B)是发挥使环氧化合物固化的作用的化合物。
作为固化剂(B),可使用公知或惯用的固化剂作为环氧树脂用固化剂。例如可举出酸酐、二羧酸、胺、聚酰胺树脂、咪唑、聚硫醇、苯酚、聚羧酸、二氰二胺(dicyanodiamide)、有机酸酰肼等。在本发明中就可靠性优异的点而言,优选选自酸酐(b-1)、二羧酸(b-2)、胺(b-3)及酚(b-4)中的至少1种化合物。
对应于固化剂(B)的官能团的分子量,例如为10~10000g/eq(优选为20~8000g/eq,更优选为20~7000g/eq,进一步优选为20~5000g/eq,特别优选为20~2000g/eq,最优选为20~1000g/eq)。
作为酸酐(b-1),例如可举出甲基四氢邻苯二甲酸酐(4-甲基四氢邻苯二甲酸酐、3-甲基四氢邻苯二甲酸酐等)、甲基六氢邻苯二甲酸酐(4-甲基六氢邻苯二甲酸酐、3-甲基六氢邻苯二甲酸酐等)、十二烯基琥珀酸酐、甲基桥亚甲基四氢邻苯二甲酸酐、邻苯二甲酸酐、马来酸酐、四氢邻苯二甲酸酐、六氢邻苯二甲酸酐、甲基环己烯二羧酸酐、苯均四酸酐、苯偏三酸酐、二苯基酮四羧酸酐、纳迪克酸酐(nadic anhydride)、甲基纳迪克酸酐、氢化甲基纳迪克酸酐、4-(4-甲基-3-戊烯基)四氢邻苯二甲酸酐、琥珀酸酐、己二酸酐、癸二酸酐、十二烷二酸酐、甲基环己烯四羧酸酐、乙烯醚-顺丁烯二酸酐共聚物、烷基苯乙烯-马来酸酐共聚物等。其中,就操作性的观点而言,优选在25℃为液态的酸酐[例如甲基四氢邻苯二甲酸酐、甲基六氢邻苯二甲酸酐、十二烯基琥珀酸酐、甲基桥亚甲基四氢邻苯二甲酸酐等]。作为酸酐固化剂,就抗破裂性特别优异的点而言,优选饱和单环烃二羧酸酐(也包括在环上键合有烷基等取代基的物质)。
作为酸酐(b-1),例如可适合使用商品名“Rikacid MH700F”(新日本理化株式会社制)、商品名“HN-5500”(日立化成工业株式会社制造)等的市售品。
作为二羧酸(b-2),例如可举出:4,4’-联苯二羧酸、2,2’-联苯二羧酸、邻苯二甲酸、间苯二甲酸、对苯二甲酸等芳香族类二羧酸;草酸、丙二酸、琥珀酸、己二酸、1,6-己烷二羧酸、1,2-环己烷二羧酸、1,3-环己烷二羧酸、1,4-环己烷二羧酸等脂肪族类二羧酸;使酸酐与多元醇化合物反应而得到的酯型二羧酸等。上述物质中,优选使酸酐与多元醇化合物反应而得到的酯型二羧酸。
作为在上述酯型二羧酸的合成中使用的酸酐,优选脂环族酸酐,其中优选4-甲基六氢邻苯二甲酸酐、六氢邻苯二甲酸酐。
作为多元醇化合物,优选二价或三价的脂肪族醇,例如可举出:乙二醇、二乙二醇、三乙二醇、1,4-丁二醇、1,6-己二醇、1,10-癸烷二醇、新戊二醇、二羟甲基丙烷、聚C1-5烷基二醇(例如聚乙二醇、聚丙二醇等)等二元脂肪族醇;甘油、三羟甲基丙烷等三元脂肪族醇类等。
上述物质中,优选二价的脂肪族醇,特别优选聚C1-5亚烷二醇。上述聚C1-5亚烷二醇的重量平均分子量例如500~2000,优选为600~1600。
作为使酸酐与多元醇化合物反应而得到的酯型二羧酸,优选以下述式(b-2-1)表示的化合物。
[化学式4]
通式(b-2-1)中,R5、R6可以相同,也可以不同,表示碳原子数1~5的烷基,其中优选甲基或乙基。m1、m2相同或不同且表示0~4的整数。L是从多元醇化合物除去2个羟基后的基团(二价基),其中优选从聚乙二醇或聚丙二醇除去2个羟基后的基团。
作为二羧酸(b-2),例如可优选使用商品名“Rikacid HF-08”(新日本理化株式会社制)等的市售品。
作为胺(b-3),例如可举出:乙二胺、二乙三胺、三乙四胺、四乙五胺、二丙二胺、二乙胺丙胺、聚丙三胺等脂肪族多胺;薄荷烯二胺(menthene diamine)、异佛尔酮二胺、双(4-胺基-3-甲基二环己基)甲烷、二胺基二环己基甲烷、双(胺甲基)环己烷、N-胺基乙基哌嗪、3,9-双(3-胺基丙基)-3,4,8,10-四氧杂螺[5,5]十一烷等脂环式多胺;间苯二胺、对苯二胺、甲苯基-2,4-二胺、甲亚苯基-2,6-二胺、1,3,5-三甲苯-2,4-二胺、3,5-二乙基甲苯基-2,4-二胺、3,5-二乙基甲苯基-2,6-二胺等单核多胺、联苯二胺、4,4-二胺基二苯基甲烷、2,5-萘二胺、2,6-萘二胺等芳香族多胺等。
作为酚(b-4),例如可举出酚醛清漆型酚醛树脂、酚醛清漆型甲酚树脂、对二甲苯改性酚醛树脂、对二甲苯/间二甲苯改性酚醛树脂等芳烷基树脂、萜烯改性酚醛树脂、二环戊二烯改性酚醛树脂、三苯酚丙烷等。
(固化催化剂(C))
本发明的固化性组合物,可含有固化催化剂(C)代替上述的固化剂(B)、或同时含有上述的固化剂(B)及固化催化剂(C)。通过使用固化催化剂(C),可使环氧化合物的固化反应进行,得到固化物。作为上述固化催化剂(C),没有特别限定,例如可使用一种或两种以上的通过施行紫外线照射或加热处理产生的阳离子种,从而使聚合开始的阳离子催化剂(阳离子聚合引发剂)。
作为通过紫外线照射而产生阳离子种的阳离子催化剂,例如可举出:六氟锑酸盐、五氟羟基锑酸盐、六氟磷酸盐、六氟砷酸盐等。作为上述阳离子催化剂,例如能够使用商品名“UVACURE1590”(Daicel.CYTEC株式会社制造)、商品名“CD-1010”、“CD-1011”、“CD-1012”(以上为美国SATOMER制造)、商品名“IRGACURE 264”(CIBA Japan株式会社制造)、商品名“CIT-1682”(日本曹达株式会社制造)等市售品。
通过施行加热处理而产生阳离子物种的阳离子催化剂,例如可举出:芳基重氮鎓盐、芳基碘鎓盐、芳基锍盐、丙二烯-离子络合物等。作为上述阳离子催化剂,例如可使用商品名“PP-33”、“CP-66”、“CP-77”(以上为ADEKA株式会社制造)、商品名“FC-509”(3M制造)、商品名“UVE1014”(G.E.制造)、商品名“San-aid SI-60L”、“San-aid SI-80L”、“San-aidSI-100L”、“San-aid SI-110L”、“San-aid SI-150L”(以上为三新化学工业株式会社制造)、商品名“CG-24-61”(CIBA Japan株式会社制造)等市售品。作为上述阳离子催化剂,可以进一步使用铝、钛等金属和乙酰乙酸或二酮类的螫合化合物与三苯基硅醇等硅醇的化合物,或者铝、钛等金属和乙酰乙酸或二酮类的螫合化合物与双酚S等酚类的化合物等。
(填料(D))
本发明的固化性组合物,也可进一步含有一种或两种以上的填料(D)。通过含有填料(D),可将固化收缩率及热线性膨胀系数抑制得更小,并且可提升翘曲的抑制效果。而且,固化性组合物含有填料(D)时,能够得到抑制填充在多孔性支持体的孔内的固化性组合物向孔外流出的效果。
作为上述填料(D),例如可举出:氧化硅(例如天然氧化硅、合成氧化硅等)、氧化铝(例如α-氧化铝等)、氧化钛、氧化锆、氧化镁、氧化铈、氧化钇、氧化钙、氧化锌、氧化铁等氧化物;碳酸钙、碳酸镁等碳酸盐;硫酸钡、硫酸铝、硫酸钙等硫酸盐;氮化铝、氮化硅、氮化钛、氮化硼等氮化物;氢氧化钙、氢氧化铝、氢氧化镁等氢氧化物;云母、滑石、高岭土、高岭土黏土、高岭石、禾乐石(halloysite)、叶蜡石、蒙脱石、绢云母、镁绿泥石(amesite)、膨土、石棉、硅灰石、海泡石(sepiolite)、金蛭石(zonolite)、沸石、水滑石、飞灰、脱水污泥、玻璃珠粒、玻璃纤维、硅藻土、硅砂、碳黑、铝硅铁粉(sendust)、铝镍钴磁铁、各种磁性氧化物(ferrite)等的磁性粉、水合石膏、明矾、三氧化锑、亚硫酸氧镁、碳化硅、钛酸钾、硅酸钙、硅酸镁、硅酸铝、磷酸镁、铜、铁等。而且,可以使用碳材料的单层或多层纳米碳管、石墨烯、氧化石墨烯等。上述填料可具有实心结构、中空结构、多孔结构等任意结构。而且,上述填料例如可以为经有机卤代硅烷、有机烷氧基硅烷、有机硅氮烷等有机硅化合物等公知的表面处理剂进行表面处理。
填料(D)的形状没有特别限定,例如可举出:球状(正球状、大致正球状、椭圆球状等)、多面体状、棒状(圆柱状、角柱状等)、平板状、鳞片状、无定形状等。
填料(D)的平均粒径例如5nm~100μm,优选为50nm~50μm,特别优选为100nm~30μm。平均粒径低于上述范围时,有粘度显著地上升且操作变得困难的倾向。另一方面,平均粒径高于上述范围时,有抗破裂性降低的倾向。而且,可以将尺寸在上述范围内的填料混合两种以上而使用,由此能够控制粘度及物性。另外,无机填料的平均粒径使用激光衍射/散射法的中值直径(d50)。
(固化促进剂)
本发明的固化性组合物,可同时含有固化剂(B)及固化促进剂。通过同时含有固化剂(B)及固化促进剂,能够得到促进固化速度的效果。作为固化促进剂,可使用公知或惯用的固化促进剂,没有特别限定,例如可举出:1,8-二氮杂双环[5.4.0]十一烯-7(DBU)、及其盐(例如苯酚盐、辛酸盐、对甲苯磺酸盐、甲酸盐、四苯基硼酸盐);1,5-二氮杂双环[4.3.0]壬烯-5(DBN)、及其盐(例如苯酚盐、辛酸盐、对甲苯磺酸盐、甲酸盐、四苯基硼酸盐);苄基二甲胺、2,4,6-三(二甲基胺甲基)苯酚、N,N-二甲基环己胺等叔胺;2-乙基-4-甲基咪唑、1-氰基乙基-2-乙基-4-甲基咪唑等咪唑类;磷酸酯、三苯基膦(TPP)等膦类;四苯基鏻四苯基硼酸盐、四苯基鏻四(对甲苯基)硼酸盐等鏻化合物;辛酸锡、辛酸锌等有机金属盐;金属螫合物等。该等可单独使用一种、或组合两种以上而使用。
作为固化促进剂,例如可适合使用商品名“U-CAT SA 506”、“U-CAT SA 102”、“U-CAT 5003”、“U-CAT 18X”、“U-CAT 12XD)”(以上为SAN-APRO株式会社制造),商品名“TPP-K”、“TPP-MK”(以上为北兴化学工业株式会社制造),商品名“PX-4ET”(日本化学工业株式会社制造)等市售品。
在本发明的固化性组合物总量中,固化性化合物(A)的含量例如30~98重量%。而且,在本发明的固化性组合物总量中,芳香族环氧化合物(例如选自表双型缩水甘油醚型环氧树脂、高分子量表双型缩水甘油醚型环氧树脂及改性表双型缩水甘油醚型环氧树脂的化合物)的含量例如30~98重量%。并且,在本发明的固化性组合物总量中,芳香族环氧化合物以外的环氧化合物所占的比例,例如20重量%以下,优选为10重量%以下,特别优选为5重量%以下,最优选为1重量%以下。
在本发明的固化性组合物所含有的环氧化合物总量中,芳香族环氧化合物(例如选自表双型缩水甘油醚型环氧树脂、高分子量表双型缩水甘油醚型环氧树脂及改性表双型缩水甘油醚型环氧树脂的化合物)所占的比例,例如60重量%以上,优选为70重量%以上,特别优选为80重量%以上,最优选为90重量%以上。另外,上限为100重量%。因此,在本发明的固化性组合物所含有的环氧化合物总量中,芳香族环氧化合物以外的环氧化合物所占的比例例如40重量%以下,优选为30重量%以下,特别优选为20重量%以下,最优选为10重量%以下。
固化性组合物含有固化剂(B)时,固化剂(B)的反应性基团相对于固化性化合物(A)的固化性基团1摩尔,优选为0.8~1.2摩尔的比例。需要说明的是,所谓“固化性基团”,指固化性化合物(A)所具有的固化性官能团。作为固化性化合物(A)的固化性基团,没有特别限定,可例示环氧基((A)为环氧化合物的情况)。而且,所谓“反应性基团”,指能够与固化性化合物(A)的“固化性基团”反应的固化剂(B)所具有的官能团。作为固化剂(B)的反应性基团,没有特别限定,可例示:作为酸酐(b-1)的反应性基团的酸酐基、作为二羧酸(b-2)的反应性基团的羧基、作为胺(b-3)的反应性基团的胺基、作为酚(b-4)的反应性基团的羟基。
在本发明的固化性组合物(填料(D)除外)总量的固化性化合物(A)及固化剂(B)的总含量所占的比例,例如80重量%以上,优选为90重量%以上,特别优选为95重量%以上。
固化剂(B)的含量低于上述范围时,固化变得不充分且固化物的强韧性有降低的倾向。另一方面,固化剂(B)的含量高于上述范围时,固化性组合物单独的固化物的极性增大,而且变得容易受到水分的影响,有时造成可靠性降低。
在本发明的固化性组合物所含有的全部固化性化合物(A)(含有固化剂(B)时,全部固化性化合物(A)与全部固化剂(B))的相对于单个官能团的分子量的加权平均值(对含有比例进行加权)(g/eq),例如180~1000,优选为200~700,特别优选为200~500,最优选为250~450,特别优选为300~450。本发明的固化性组合物,选择含有固化性化合物(A)(含有固化剂(B)时为固化性化合物(A)与固化剂(B)),使加权平均值成在上述范围中,由于适当地具有交联点间距离而具有柔软性且能够得到具有抗破裂性优异的固化物的点出发,优选。加权平均值低于上述范围时,有柔软性降低且抗破裂性降低的倾向。另一方面,加权平均值高于上述范围时,有固化树脂的密度较低且难以得到充分的强韧性和耐候性的倾向。需要说明的是,相对于环氧化合物的官能团的分子量,指环氧当量。而且,作为相对于固化剂的酸酐(b-1)的官能团的分子量,指酸酐基团当量;相对于二羧酸(b-2)的官能团的分子量,指羧基当量;相对于胺(b-3)的官能团的分子量,指胺当量;相对于酚(b-4)的官能团的分子量,指羟基当量。
固化催化剂(C)的含量没有特别限定,相对于在固化性组合物中所含有的固化性化合物(A)100重量份,例如优选为含有0.1~10重量份的比例;相对于在固化性组合物中所含有的环氧化合物的总量(100重量份),例如0.01~15重量份,优选为0.01~12重量份,更优选为0.05~10重量份,特别优选为0.1~10重量份。通过在上述范围内使用固化催化剂(C),可得到耐热性、耐候性优异的固化物。
相对于在固化性组合物中所含有的固化性化合物(含有两种以上时为其总量)100重量份,填料(D)的含量例如50重量份以下(例如1~50重量份),优选为45重量份以下,特别优选为40重量份以下。填料(D)的含量过剩时,固化性组合物单独的固化物的Tg变高且柔软性降低,有抗破裂性降低的倾向。
固化促进剂的含量没有特别限定,相对于在固化性组合物中所含有的环氧化合物100重量份,例如为3重量份以下(例如0.1~3重量份),优选为0.2~3重量份,特别优选为0.25~2.5重量份。
(其他成分)
本发明的固化性组合物除了上述成分以外,可以根据需要而含有一种或两种以上的其它成分。
本发明的固化性组合物可以含有环氧化合物以外的固化性化合物,例如可以含有氧杂环丁烷化合物等阳离子固化性化合物、(甲基)丙烯酸酯、胺甲酸酯(甲基)丙烯酸酯等自由基固化性化合物。
本发明的固化性组合物也能够进一步含有例如稀释剂、消泡剂、流平剂、硅烷偶联剂、表面活性剂、阻燃剂、着色剂、增塑剂、抗静电剂、脱模剂、抗氧化剂、紫外线吸收剂、光稳定剂、离子吸附物、萤光物等。
而且,使用酸酐作为固化剂(B)时,酸酐与乙二醇、二乙二醇、丙二醇、甘油等含羟基的化合物一起使用,能够得到促进固化反应的效果的点出发,优选。相对于酸酐100重量份,含羟基的化合物的含量例如0.1~15重量份,优选为0.5~10重量份。
本发明的固化性组合物可通过混合上述成分来制备。混合可使用自转公转式搅拌脱泡装置、均质机、行星式搅拌机、三辊研磨机、珠磨机等通常已知的混合用机器。而且,各成分可同时混合,也可逐次混合。
本发明的固化性组合物单独的固化物(不包含多孔性支持体)的玻璃化转变温度(Tg),例如-60~100℃(Tg的上限优选为50℃,特别优选为40℃,最优选为25℃。Tg的下限优选为-40℃,更优选为-30℃,又更优选为-20℃,进一步优选为-10℃,特别优选为0℃,最优选为5℃,特别优选为10℃),在上述玻璃化转变温度以上的温度(例如-10~220℃,优选为0~220℃,特别优选为10~200℃,最优选为20~220℃,特别优选为50~220℃)范围的至少1点的本发明的固化性组合物单独的固化物(不包含多孔性支持体)的热线性膨胀系数,例如100ppm/K以上(例如100~700ppm/K,优选为200~500ppm/K,特别优选为300~500ppm/K)。
[片状预浸料]
本发明的片状预浸料具有上述多孔性支持体的孔内填充有上述固化性组合物的结构。由于本发明所使用的固化性组合物单体的固化物如上所述,玻璃化转变温度较低且较柔软,因此具有优异的抗破裂性。而且,形成上述的柔软的(特别是在100℃以上的高温区域为柔软的)固化物的固化性组合物,虽然具有被填充在多孔性支持体的孔内的构成,但由于上述固化性组合物无法将多孔性支持体推开而膨胀,故结果可将热线性膨胀系数抑制为较小,且可防止产生翘曲。
本发明的片状预浸料,例如可通过使由溶剂(例如2-丁酮等)稀释上述固化性组合物而得到的物质含浸于上述多孔性支持体,然后,使其干燥并将溶剂除去,根据需要而使其进行半固化(使固化性化合物的一部分固化)来制造。
作为含浸固化性组合物的方法,没有特别限制,例如可举出将多孔性支持体浸渍在固化性组合物中的方法等。浸渍时的温度,例如25~60℃左右。浸渍时间,例如30秒钟~30分钟左右。就能够得到抑制起泡的残留且促进固化性组合物的填充的效果而言,浸渍优选在减压或加压环境下进行。
含浸后的干燥及半固化条件,优选根据固化剂的种类适当地变更而进行。例如使用酸酐或苯酚作为固化剂时,可通过以小于100℃(例如25℃以上且小于100℃)的温度加热1分钟~1小时左右来进行。使用胺作为固化剂时,优选在较低的温度下进行。加热温度和加热时间高于上述范围时,由于被填充在多孔性支持体的固化性组合物的固化反应过度地进行,有时难以用作密封材料。
在本发明的片状预浸料总体积中,多孔性支持体所占的比例例如10~90vol%,优选为20~70vol%,特别优选为30~70vol%,最优选为30~50vol%。即,在本发明的片状预浸料总体积中,固化性组合物所占的比例例如10~90vol%,优选为30~80vol%,特别优选为30~70vol%,最优选为50~70vol%。多孔性支持体所占的比率若高于上述范围,则难以含浸充分量的上述固化性组合物,从而有不易得到表面平滑性的倾向。另一方面,固化性组合物高于上述范围时,则无法充分地得到通过多孔性支持体产生的增强效果,从而有难以将固化收缩率及热线性膨胀系数抑制为较小的倾向。
本发明的片状预浸料,通过施行加热处理来形成固化物。加热处理条件没有特别限定,优选加热温度为40~300℃,优选为60~250℃。而且,加热时间可以根据加热温度而适当地调节,而没有特别限定,优选1~10小时,更优选1~5小时。在上述加热处理中,加热温度可设为恒定,也可设为连续地或阶段性地改变。
本发明的片状预浸料的固化物的玻璃化转变温度(Tg)为-60℃以上且100℃以下(-60~100℃),优选为0~90℃,更优选为5~80℃,进一步更优选为10~75℃,特别优选为10~60℃,最优选为10~50℃,进一步更优选为10~40℃,更特别优选为15~40℃。由于本发明的片状预浸料的固化物具有上述Tg,因此具有适当的柔软性,且抗破裂性优异。另外,固化物的玻璃化转变温度能够以实施例所记载的方法求得。
本发明的片状预浸料的固化物的热线性膨胀系数[例如在-20℃~300℃,优选为-10~300℃,特别优选为0~300℃]的热线性膨胀系数]例如55ppm/K以下(例如-1~55ppm/K),优选为50ppm/K以下,更优选为45ppm/K以下,进一步更优选为25ppm/K以下,特别优选为20ppm/K以下。因此,能够抑制因热所致的膨胀或收缩,并且可抑制产生翘曲。即,抗翘曲性优异。
本发明的片状预浸料,可优选用作压缩成形用密封材料(特别是FOWLP用密封材料)。
使用本发明的片状预浸料的FOWLP的代表性制造方法如下述(参照第1图)。
工序I:将暂时固定胶带贴附在支持体,将半导体芯片经由上述暂时固定胶带贴附在支持体;
工序II:使用本发明的片状预浸料对半导体芯片进行密封;
工序III:将支持体剥离;
工序IV:进行再布线、电极形成及切割(dicing)而得到半导体封装。
在上述工序II中,作为使用本发明的片状预浸料而将芯片密封的方法,例如可如下进行:将本发明的片状预浸料贴合在芯片,使用表面平坦化用基板等进行压缩(例如以0.1~5MPa按压)且通过使用上述方法施行加热处理。
在工序IV的再布线和电极形成,可以使用众所公知惯用的方法而进行。再布线和电极形成,在约200℃的高温环境下进行,本发明的片状预浸料的固化物的热线性膨胀系数为上述范围,因此可抑制与半导体芯片的热膨胀率之差,而且可抑制来自与半导体芯片的热膨胀率之差的应力所引起的翘曲和破裂。
而且,将本发明的片状预浸料贴合在例如已薄化至100μm以下的硅芯片及基板的至少一面上,并进行固化,由此可发挥防止硅芯片和基板的翘曲的效果。因此,本发明的片状预浸料可以用作薄化硅芯片和薄化基板的抗翘曲材料。
实施例
以下,通过实施例进一步具体地说明本发明,但是本发明不限定于这些实施例。
制备例1:支撑体的制备(纤维素无纺布的制备)
将微小纤维CELISH KY110N(Daicel株式会社制)的浆料稀释成为0.2重量%,使用带有减压装置的抄纸机(株式会社东洋精机制作所制造,标准方型机器),将No.5C滤纸作为滤布进行抄纸,得到湿润状态的纤维素无纺布。
将吸墨纸重叠在得到的湿润状态的纤维素无纺布的两个表面上,以0.2MPa的压力加压1分钟。接着,以0.2MPa的压力加压1分钟,再贴附至表面温度设定为100℃的滚筒干燥机(熊谷理机工业株式会社制)并干燥120秒钟,得到纤维素无纺布(孔隙率:60vol%、单位面积重量9.9g/m2、热线性膨胀系数:5ppm/K、厚度25μm)。
实施例1、实施例2、实施例3、实施例9、实施例10、比较例1~比较例3
(片状预浸料的制备)
使用表1所记载的处方制备固化性组合物。
将制备例1所得的纤维素无纺布在减压下浸渍在得到的固化性组合物中,使固化性组合物含浸在纤维素无纺布中,制得片状预浸料(固化性组合物所占的比率:65vol%)。另外,在实施例9使用以与制备例1相同的方法而得到的纤维素无纺布(孔隙率:60vol%、单位面积9.9g/m2、热线性膨胀系数:5ppm/K、厚度50μm)。而且,在实施例10中,使用玻璃布取代纤维素无纺布。
而且,对于实施例1所使用的固化性组合物单独固化而得到的固化物,通过下述方法测定玻璃化转变温度及热线性膨胀系数时,Tg:17.5℃、热线性膨胀系数(α1):65.8ppm/K、热线性膨胀系数(α2):466.8ppm/K。
(片状预浸料的评价)
将所得到的片状预浸料夹入涂布有脱模剂的玻璃,并且在表1中记载的固化条件下加热而得到固化物,并依照下述方法测定得到的固化物的玻璃化转变温度及热线性膨胀系数。
而且,将4个10mm见方的硅芯片再配置在50mm见方的玻璃基板上,且使用上述片状预浸料进行覆盖,通过加压成型(compression molding)(在经表1所记载的初期固化条件进行加热后的状态,以1MPa按压)来进行硅芯片的密封。然后,将内包硅芯片的半导体封装体从基板剥下,并以下述方法评估其抗翘曲性及抗破裂性。
实施例4、实施例5、实施例6、实施例7、实施例8
使用表1所记载的处方制备固化性组合物,混合甲基乙基酮,使固体成分浓度成为40%,得到固化性组合物。
使该固化性组合物含浸在制备例1中得到的纤维素无纺布,在减压下除去溶剂,制得片状预浸料。
对于得到的片状预浸料,使用与实施例1相同的方法进行评估。
实施例11、实施例12
按照表1记载的处方将填料及环氧树脂填料于擂溃机(石川工场株式会社制造)并混炼30分钟,得到高分散有填料的环氧树脂。然后,添加酸酐,并添加乙二醇及催化剂,进行混炼。最后,添加甲基乙基酮使固体成分浓度成为40%,得到固化性组合物。
使该固化性组合物含浸在制备例1中得到的纤维素无纺布,在减压下除去溶剂,制得片状预浸料。
对于所得的片状预浸料,以与实施例1相同的方法进行评估。
(玻璃化转变温度(Tg)、比Tg低的温度区域的热线性膨胀系数(α1)、比Tg高的温度区域的热线性膨胀系数(α2))
固化物的玻璃化转变温度及热线性膨胀系数,以下述条件进行测定。另外,均是采用第二次加热(2nd-heating)的测定值。
试片尺寸:初期长度10mm×宽度3.5mm×厚度0.035mm
测定装置:热机械分析装置(Exstar TMA/SS7100、日立High-Technologies株式会社制造)
测定模式:拉伸、定载重测定(40mN)
测定气体环境:氮
温度条件:第一次加热(1st-heating) 从-60℃起~120℃、5℃/分钟
冷却(cooling) 从120℃起~-60℃、20℃/分钟
第二次加热(2nd-heating) 从-60℃起~220℃、5℃/分钟
(抗翘曲性)
测定在25℃、150℃、275℃下的半导体封装的翘曲量(参照第2图),以下述基准进行抗翘曲性评估。
○:在25℃、150℃、275℃中的温度下,翘曲量均为10μm以下
△:在25℃、150℃、275℃的至少一个温度下,翘曲量超过10μm且50μm以下
×:在25℃、150℃、275℃的至少一个温度下,翘曲量超过50μm
(抗破裂性)
对半导体封装体实施-25℃~100℃的热冲击试验(100次),对于实施试验后的半导体封装,通过目视观察有无破裂,且以下述基准评估抗破裂性。
○:无破裂
×:有破裂
<环氧化合物>
.YD-128:双酚A型缩水甘油醚(环氧当量190,粘度13600mPa·s/25℃),环氧当量188.6,新日铁住金化学株式会社制造
.CELLOXIDE 2021P:3,4-环氧环己基甲基(3,4-环氧基)环己烷羧酸酯,环氧当量130,Daicel株式会社制造
.EXA-4850-150:改性表双型缩水甘油醚型环氧树脂,环氧当量:433,商品名“EPICLON EXA-4850-150”,DIC株式会社制造
.EXA-4850-1000:下述式(ii-1)表示的改性表双型缩水甘油醚型环氧树脂,环氧当量:350,商品名“EPICLON EXA-4850-1000”,DIC株式会社制造
[化学式5]
<固化剂>
.Rikacid MH-700:甲基六氢邻苯二甲酸酐,酸酐基当量164.5,新日本理化株式会社制造
.Rikacid HF-08:脂环族酸酐与聚烷基二醇形成的酯(二羧酸),羧基当量672.7,新日本理化株式会社制造
.TD2091:苯酚酚醛清漆,羟基当量104.0,DIC株式会社制造
.TETA:三乙基四胺,胺当量23.4,三井化学FINE株式会社制造
.D-400:聚氧化烯烃二胺,胺当量107.0,三井化学FINE株式会社制造
<稀释剂>
.EG:乙二醇,和光纯药工业株式会社制造
<固化促进剂>
.U-CAT 12XD:特殊胺型催化剂,SAN-APRO株式会社制造
.TPP:三苯基膦,和光纯药工业株式会社制
<固化催化剂>
.2E4MIZ:2-乙基-4-甲基咪唑,和光纯药工业株式会社制造
<填料>
.氧化硅填料:粒径3μm以下,日本电气硝子株式会社制造
.纳米碳管:长度:10μm以上,直径:20~45nm,GLONATECH公司制造
<多孔性支撑体>
.玻璃布:孔隙率:62vol%,单位面积重量24g/m2,热线性膨胀系数:3ppm/k,厚度25μm,商品名“1037”、东洋纺株式会社制造
以下,对以上内容进行总结,附记本发明的技术特征及其变异。
[1]一种片状预浸料,其具有包含热线性膨胀系数为10ppm/K以下的材料的片状多孔性支持体的孔内填充有下述固化性组合物的构成,该片状预浸料的固化物的玻璃化转变温度为-60℃以上且100℃以下;固化性组合物:是含有固化性化合物(A)、固化剂(B)和/或固化催化剂(C)的组合物,其中,所述组合物中的(A)总量的50重量%以上为环氧当量140~3000g/eq的环氧化合物。
[2]根据[1]所述的片状预浸料,其中,片状预浸料的固化物通过施行加热处理而形成,加热温度为40~300℃,加热时间为1~10小时。
[3]根据[1]或[2]所述的片状预浸料,其中,片状多孔性支持体包含热线性膨胀系数为7ppm/K以下(特别优选为5ppm/K以下)的材料。
[4]根据[1]~[3]项中任一项所述的片状预浸料,其中,热线性膨胀系数为10ppm/K以下的材料是纸、纤维素、玻璃纤维或液晶材料。
[5]根据[1]~[4]项中任一项所述的片状预浸料,其中,多孔性支持体的孔隙率为90~10vol%(优选为80~30vol%,特别优选为70~30vol%,最优选为70~50vol%),多孔性支持体的厚度为5~500μm(下限优选为10μm,特别优选为15μm,最优选为20μm,上限优选为300μm,更优选为200μm,特别优选为100μm,最优选为75μm)。
[6]根据[1]~[5]项中任一项所述的片状预浸料,其中,固化性化合物(A)以(A)总量的50重量%以上(优选为70重量%以上,特别优选为80重量%以上,最优选为90重量%以上,另外,上限为100重量)含有环氧当量(g/eq)为140~3000(优选为170~1000,更优选为180~1000,特别优选为180~500)的环氧化合物。
[7]根据[1]~[6]项中任一项所述的片状预浸料,其中,固化性组合物含有选自脂环式环氧化合物、芳香族环氧化合物(例如表双型缩水甘油醚型环氧树脂、高分子量表双型缩水甘油醚型环氧树脂或改性表双型缩水甘油醚型环氧树脂)及脂肪族环氧化合物中的至少一种作为环氧化合物。
[8]根据[7]所述的片状预浸料,其中,改性表双型缩水甘油醚型环氧树脂为上述式(ii)表示的化合物(式中,R1~R4相同或不同,表示氢原子或烃基;k表示1以上的整数,L1表示低极性键合基,L2表示柔软性骨架)。
[9]根据[1]~[8]项中任一项所述的片状预浸料,其中,固化剂(B)选自酸酐(b-1)、二羧酸(b-2)、胺(b-3)及酚(b-4)中的至少一种化合物。
[10]根据[1]~[9]项中任一项所述的片状预浸料,其中,固化性组合物总量中的固化性化合物(A)的含量为30~98重量%,在固化性组合物总量中的芳香族环氧化合物(例如表双型缩水甘油醚型环氧树脂、高分子量表双型缩水甘油醚型环氧树脂及改性表双型缩水甘油醚型环氧树脂的化合物)的含量为30~98重量%,在固化性组合物总量中,芳香族环氧化合物以外的环氧化合物所占的比率为20重量%以下(优选为10重量%以下,特别优选为5重量%以下,最优选为1重量%以下)。
[11]根据[1]~[10]项中任一项所述的片状预浸料,其中,在固化性组合物所含有的环氧化合物总量中,芳香族环氧化合物(例如选自表双型缩水甘油醚型环氧树脂、高分子量表双型缩水甘油醚型环氧树脂及改性表双型缩水甘油醚型环氧树脂的化合物)所占的比率为60重量%以上(优选为70重量%以上,特别优选为80重量%以上,最优选为90重量%以上;且上限为100重量%)。
[12]根据[1]~[11]项中任一项所述的片状预浸料,其中,固化性组合物含有固化剂(B),并且使固化剂(B)成为下述比例:
相对于固化性化合物(A)的固化性基团1摩尔,固化剂(B)的反应性基团为0.8~1.2摩尔。
[13]根据[1]~[12]项中任一项所述的片状预浸料,其中,固化性组合物含有的固化性化合物(A)及固化催化剂(C),相对于上述(A)100重量份,(C)为0.1~10重量份。
[14]根据[1]~[13]项中任一项所述的片状预浸料,其中,固化性组合物所含有的全部固化性化合物(A)(含有固化剂(B)时,为全部固化性化合物(A)与全部固化剂(B))的相对于单个官能团的分子量的加权平均值为180~1000(优选为200~700,特别优选为200~500,最优选为250~450,特别优选为300~450)g/eq。
[15]根据[1]~[14]项中任一项所述的片状预浸料,其中,固化性组合物的固化物的热线性膨胀系数为100ppm/K以上(例如100~700ppm/K,优选为200~500ppm/K,特别优选为300~500ppm/K)。
[16]根据[1]~[15]项中任一项所述的片状预浸料,其中,片状预浸料的固化物的热线性膨胀系数为55ppm/K以下(例如-1~55ppm/K,优选为50ppm/K以下,优选为45ppm/K以下,更优选为25ppm/K以下,特别优选为20ppm/K以下)。
[17]根据[1]~[16]项中任一项所述的片状预浸料,其中,固化性组合物(填料(D)除外)总量中的固化性化合物(A)及固化剂(B)的合计含量所占的比率为80重量%以上(优选为90重量%以上,特别优选为95重量%以上)。
[18]根据[1]~[17]项中任一项所述的片状预浸料,其中,相对于固化性化合物(A)100重量份,固化性组合物中的填料(D)的含量为50重量份以下(例如1~50重量份,优选为45重量份以下,特别优选为40重量份以下)。
[19]根据[1]~[18]项中任一项所述的片状预浸料,其中,固化物的玻璃化转变温度(Tg)为-60~100℃(Tg的上限优选为50℃,特别优选为40℃,最优选为25℃,下限优选为-40℃,更优选为-30℃,又更优选为-20℃,复又更优选为-10℃,特别优选为0℃,最优选为5℃,尤特别优选为10℃)。
[20]根据[1]~[19]项中任一项所述的片状预浸料,其中,在玻璃化转变温度以上的温度(例如-10~220℃,优选为0~220℃,特别优选为10~200℃,最优选为20~220℃,特别优选为50~220℃)范围的至少1点的固化物的热线性膨胀系数为100ppm/K以上(例如100~700ppm/K,优选为200~500ppm/K,特别优选为300~500ppm/K)。
[21]根据[1]~[20]项中任一项所述的片状预浸料,其中,片状多孔性支持体的厚度为5~500μm。
[22]根据[1]~[21]项中任一项所述的片状预浸料,其是压缩成形用密封材料。
[23]根据[1]~[22]项中任一项所述的片状预浸料,其是扇出型晶圆级封装用密封材料。
[24]根据[1]~[23]项中任一项所述的片状预浸料,其是厚度为100μm以下的薄化硅芯片或薄化基板的抗翘曲材料。
工业实用性
本发明的片状预浸料,通过热固化而具有适当的柔软性,且由于热所致的收缩率和膨胀率较低,可以形成可发挥优异的抗翘曲性及抗破裂性的固化物。因此,本发明的片状预浸料可优选用作FOWLP用密封材料和基板的抗翘曲材料。
符号说明
1 支撑体
2 临时固定胶带
3 芯片
4 片状预浸料
5 表面平整基板
6 半导体封装
7 翘曲量
Claims (10)
1.一种片状预浸料,其具有如下结构:包含热线性膨胀系数为10ppm/K以下的材料的片状多孔性支持体的孔内填充有下述固化性组合物,
该片状预浸料的固化物的玻璃化转变温度为-60℃以上且100℃以下,
固化性组合物是:包含固化性化合物(A)、固化剂(B)和/或固化催化剂(C)的组合物,其中,(A)总量的50重量%以上是环氧当量为140~3000g/eq的环氧化合物。
2.根据权利要求1所述的片状预浸料,其中,固化性组合物含有固化剂(B),并且使固化剂(B)的比例如下:
相对于固化性化合物(A)的固化性基团1摩尔,固化剂(B)的反应性基团为0.8~1.2摩尔。
3.根据权利要求1或2所述的片状预浸料,其中,固化性组合物含有固化性化合物(A)及固化催化剂(C),并且相对于上述(A)100重量份,(C)的比例为0.1~10重量份。
4.根据权利要求1~3中任一项所述的片状预浸料,其中,固化性组合物所包含的全部固化性化合物(A)(含有固化剂(B)时,为全部固化性化合物(A)和全部固化剂(B))的相对于单个官能团的分子量的加权平均值为180~1000g/eq。
5.根据权利要求1~4中任一项所述的片状预浸料,其中,固化性组合物的固化物的热线性膨胀系数为100ppm/K以上,且片状预浸料的固化物的热线性膨胀系数为55ppm/K以下。
6.根据权利要求1~5中任一项所述的片状预浸料,其中,固化性组合物含有相对于固化性化合物(A)100重量份为1~50重量份的填料(D)。
7.根据权利要求1~6中任一项所述的片状预浸料,其中,片状多孔性支持体的厚度为5~500μm。
8.根据权利要求1~7中任一项所述的片状预浸料,其是压缩成形用密封材料。
9.根据权利要求1~7中任一项所述的片状预浸料,其是扇出型晶圆级封装用密封材料。
10.根据权利要求1~7中任一项所述的片状预浸料,其是厚度100μm以下的薄化硅芯片或薄化基板的抗翘曲材料。
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