TWI715620B - 樹脂組合物 - Google Patents
樹脂組合物 Download PDFInfo
- Publication number
- TWI715620B TWI715620B TW105127397A TW105127397A TWI715620B TW I715620 B TWI715620 B TW I715620B TW 105127397 A TW105127397 A TW 105127397A TW 105127397 A TW105127397 A TW 105127397A TW I715620 B TWI715620 B TW I715620B
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- Prior art keywords
- ene
- resin composition
- resin
- hept
- acrylate
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- 239000011342 resin composition Substances 0.000 title claims abstract description 91
- -1 quinonediazide compound Chemical class 0.000 claims abstract description 146
- 229920005989 resin Polymers 0.000 claims abstract description 109
- 239000011347 resin Substances 0.000 claims abstract description 109
- 239000003431 cross linking reagent Substances 0.000 claims abstract description 39
- 239000013034 phenoxy resin Substances 0.000 claims abstract description 34
- 229920006287 phenoxy resin Polymers 0.000 claims abstract description 34
- 125000002887 hydroxy group Chemical group [H]O* 0.000 claims abstract description 30
- 239000011230 binding agent Substances 0.000 claims abstract description 27
- 150000001875 compounds Chemical class 0.000 claims description 61
- 229920000089 Cyclic olefin copolymer Polymers 0.000 claims description 25
- 239000004593 Epoxy Substances 0.000 claims description 24
- 125000004849 alkoxymethyl group Chemical group 0.000 claims description 18
- IISBACLAFKSPIT-UHFFFAOYSA-N bisphenol A Chemical group C=1C=C(O)C=CC=1C(C)(C)C1=CC=C(O)C=C1 IISBACLAFKSPIT-UHFFFAOYSA-N 0.000 claims description 14
- 125000004029 hydroxymethyl group Chemical group [H]OC([H])([H])* 0.000 claims description 13
- 239000007787 solid Substances 0.000 claims description 13
- 239000000945 filler Substances 0.000 claims description 11
- 125000002723 alicyclic group Chemical group 0.000 claims description 8
- 125000004122 cyclic group Chemical group 0.000 claims description 2
- 150000002632 lipids Chemical class 0.000 claims 1
- 239000010408 film Substances 0.000 description 90
- NIXOWILDQLNWCW-UHFFFAOYSA-M Acrylate Chemical compound [O-]C(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-M 0.000 description 80
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- 239000000126 substance Substances 0.000 description 29
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 description 20
- 229910000679 solder Inorganic materials 0.000 description 18
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- 238000010438 heat treatment Methods 0.000 description 15
- 125000000217 alkyl group Chemical group 0.000 description 14
- 229920000642 polymer Polymers 0.000 description 14
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 13
- 230000005855 radiation Effects 0.000 description 13
- 125000003118 aryl group Chemical group 0.000 description 12
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 11
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 10
- 238000002156 mixing Methods 0.000 description 10
- CERQOIWHTDAKMF-UHFFFAOYSA-N Methacrylic acid Chemical compound CC(=C)C(O)=O CERQOIWHTDAKMF-UHFFFAOYSA-N 0.000 description 9
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- ISWSIDIOOBJBQZ-UHFFFAOYSA-N phenol group Chemical group C1(=CC=CC=C1)O ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 7
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- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
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- PAPBSGBWRJIAAV-UHFFFAOYSA-N ε-Caprolactone Chemical class O=C1CCCCCO1 PAPBSGBWRJIAAV-UHFFFAOYSA-N 0.000 description 5
- YBYIRNPNPLQARY-UHFFFAOYSA-N 1H-indene Chemical compound C1=CC=C2CC=CC2=C1 YBYIRNPNPLQARY-UHFFFAOYSA-N 0.000 description 4
- CDAWCLOXVUBKRW-UHFFFAOYSA-N 2-aminophenol Chemical compound NC1=CC=CC=C1O CDAWCLOXVUBKRW-UHFFFAOYSA-N 0.000 description 4
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- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 description 4
- 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
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- VZCYOOQTPOCHFL-OWOJBTEDSA-N Fumaric acid Chemical compound OC(=O)\C=C\C(O)=O VZCYOOQTPOCHFL-OWOJBTEDSA-N 0.000 description 4
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 4
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- XXROGKLTLUQVRX-UHFFFAOYSA-N allyl alcohol Chemical compound OCC=C XXROGKLTLUQVRX-UHFFFAOYSA-N 0.000 description 4
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- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 238000007796 conventional method Methods 0.000 description 4
- 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 4
- BGTOWKSIORTVQH-UHFFFAOYSA-N cyclopentanone Chemical compound O=C1CCCC1 BGTOWKSIORTVQH-UHFFFAOYSA-N 0.000 description 4
- 238000001035 drying Methods 0.000 description 4
- RTZKZFJDLAIYFH-UHFFFAOYSA-N ether Substances CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 4
- JBFHTYHTHYHCDJ-UHFFFAOYSA-N gamma-caprolactone Chemical compound CCC1CCC(=O)O1 JBFHTYHTHYHCDJ-UHFFFAOYSA-N 0.000 description 4
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 4
- 239000011261 inert gas Substances 0.000 description 4
- 125000001449 isopropyl group Chemical group [H]C([H])([H])C([H])(*)C([H])([H])[H] 0.000 description 4
- 238000003475 lamination Methods 0.000 description 4
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- MKUWVMRNQOOSAT-UHFFFAOYSA-N methylvinylmethanol Natural products CC(O)C=C MKUWVMRNQOOSAT-UHFFFAOYSA-N 0.000 description 4
- 125000001624 naphthyl group Chemical group 0.000 description 4
- 125000004430 oxygen atom Chemical group O* 0.000 description 4
- 239000002245 particle Substances 0.000 description 4
- 229960003742 phenol Drugs 0.000 description 4
- 125000000951 phenoxy group Chemical group [H]C1=C([H])C([H])=C(O*)C([H])=C1[H] 0.000 description 4
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 description 4
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- 239000005977 Ethylene Substances 0.000 description 3
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 3
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- JCVQKRGIASEUKR-UHFFFAOYSA-N triethoxy(phenyl)silane Chemical compound CCO[Si](OCC)(OCC)C1=CC=CC=C1 JCVQKRGIASEUKR-UHFFFAOYSA-N 0.000 description 1
- NBXZNTLFQLUFES-UHFFFAOYSA-N triethoxy(propyl)silane Chemical compound CCC[Si](OCC)(OCC)OCC NBXZNTLFQLUFES-UHFFFAOYSA-N 0.000 description 1
- BOVWGKNFLVZRDU-UHFFFAOYSA-N triethoxy(trifluoromethyl)silane Chemical compound CCO[Si](OCC)(OCC)C(F)(F)F BOVWGKNFLVZRDU-UHFFFAOYSA-N 0.000 description 1
- 125000002023 trifluoromethyl group Chemical group FC(F)(F)* 0.000 description 1
- SRPWOOOHEPICQU-UHFFFAOYSA-N trimellitic anhydride Chemical compound OC(=O)C1=CC=C2C(=O)OC(=O)C2=C1 SRPWOOOHEPICQU-UHFFFAOYSA-N 0.000 description 1
- JLGNHOJUQFHYEZ-UHFFFAOYSA-N trimethoxy(3,3,3-trifluoropropyl)silane Chemical compound CO[Si](OC)(OC)CCC(F)(F)F JLGNHOJUQFHYEZ-UHFFFAOYSA-N 0.000 description 1
- ZNOCGWVLWPVKAO-UHFFFAOYSA-N trimethoxy(phenyl)silane Chemical compound CO[Si](OC)(OC)C1=CC=CC=C1 ZNOCGWVLWPVKAO-UHFFFAOYSA-N 0.000 description 1
- HQYALQRYBUJWDH-UHFFFAOYSA-N trimethoxy(propyl)silane Chemical compound CCC[Si](OC)(OC)OC HQYALQRYBUJWDH-UHFFFAOYSA-N 0.000 description 1
- ORVBHOQTQDOUIW-UHFFFAOYSA-N trimethoxy(trifluoromethyl)silane Chemical compound CO[Si](OC)(OC)C(F)(F)F ORVBHOQTQDOUIW-UHFFFAOYSA-N 0.000 description 1
- BPSIOYPQMFLKFR-UHFFFAOYSA-N trimethoxy-[3-(oxiran-2-ylmethoxy)propyl]silane Chemical compound CO[Si](OC)(OC)CCCOCC1CO1 BPSIOYPQMFLKFR-UHFFFAOYSA-N 0.000 description 1
- LTOKKZDSYQQAHL-UHFFFAOYSA-N trimethoxy-[4-(oxiran-2-yl)butyl]silane Chemical compound CO[Si](OC)(OC)CCCCC1CO1 LTOKKZDSYQQAHL-UHFFFAOYSA-N 0.000 description 1
- YUYCVXFAYWRXLS-UHFFFAOYSA-N trimethoxysilane Chemical compound CO[SiH](OC)OC YUYCVXFAYWRXLS-UHFFFAOYSA-N 0.000 description 1
- 125000002948 undecyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- XSQUKJJJFZCRTK-UHFFFAOYSA-N urea group Chemical group NC(=O)N XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 1
- NQPDZGIKBAWPEJ-UHFFFAOYSA-N valeric acid Chemical compound CCCCC(O)=O NQPDZGIKBAWPEJ-UHFFFAOYSA-N 0.000 description 1
- 229910052724 xenon Inorganic materials 0.000 description 1
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 description 1
- 239000008096 xylene Substances 0.000 description 1
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Abstract
提供一種含有黏結劑樹脂(A)、羥基當量為300以上的苯氧基樹脂(B)及交聯劑(C)之樹脂組合物。本發明的樹脂組合物更含有光酸產生劑(D)為佳,光酸產生劑(D)以醌二疊氮化合物為較佳。
Description
本發明係有關於一種具備樹脂組合物及由該樹脂組合物所構成的樹脂膜之電子元件,更詳言之,係有關於一種能夠供給具有優異的耐熱性、對基板的密著性、焊料耐熱性、及耐熱衝擊性的樹脂膜之樹脂組合物及具備由該樹脂組合物所構成的樹脂膜之電子元件。
有機EL元件、液晶顯示元件等的各種顯示元件、積體電路元件、固態攝影元件、彩色濾光片、黑色矩陣等的電子元件,係設置各種樹脂膜,例如表面保護膜以防止其劣化和損傷,平坦化膜以將元件表面和配線平坦化,及層間絕緣膜,使設置為層狀的配線之間絕緣。
先前,作為用以形成該等樹脂膜之樹脂材料,係廣泛地應用環氧樹脂、聚醯亞胺、聚苯並噁唑等的熱硬化性樹脂材料。近年來,隨著配線和裝置的高密度化,該等樹脂材料亦被要求開發一種具有優異的低介電性等的電特性之新穎樹脂材料。
為了因應該等要求,例如專利文獻1係揭示一種樹脂組合物,其係含有具有質子性極性基的環狀烯烴聚合物(A)、交聯劑(B)及放射線感應化合物(C);相對於環狀烯烴聚合
物(A)100重量份,放射線感應化合物(C)的含量為10~45重量份。但是,使用該專利文獻1所記載的放射線感應樹脂組合物時,雖然具有優異的低介電性等的電特性且能夠形成具有優異的耐熱性之樹脂膜,但是對基板的密著性、焊料耐熱性、耐熱衝擊性為不充分,因此被期望改善該等特性。
先前技術文獻
專利文獻
[專利文獻1]日本特開2009-295374號公報
本發明之目的,係提供一種能夠供給具有優異的耐熱性、對基板的密著性、焊料耐熱性、及耐熱衝擊性的樹脂膜之樹脂組合物、及具備由此種樹脂組合物所構成的樹脂膜之電子元件。
為了達成上述目的,本發明者等專心研究之結果,發現藉由在黏結劑樹脂混合羥基量為特定範圍之苯氧基樹脂及交聯劑而得到之樹脂組合物,能夠達成上述目的而完成了本發明。
亦即,依照本發明,能夠提供[1]一種樹脂組合物,係含有黏結劑樹脂(A)、羥基當量為300以上的苯氧基樹脂(B)及交聯劑(C),[2]如前述[1]所述之樹脂組合物,其中相對於形成前述樹脂組合物之固體成分全體,以80重量%以下的含量含有填料,
[3]如前述[2]所述之樹脂組合物,其中相對於形成前述樹脂組合物之固體成分全體,前述填料的含量為0重量%,[4]如前述[1]至[3]項中任一項所述之樹脂組合物,其中前述交聯劑(C)係在分子內含有2個以上的烷氧基甲基或羥甲基之化合物,[5]如前述[1]至[3]項中任一項所述之樹脂組合物,其中前述交聯劑(C)為脂環式環氧化合物,[6]如前述[1]至[3]項中任一項所述之樹脂組合物,其中前述交聯劑(C)係在分子內含有2個以上的烷氧基甲基或羥甲基之化合物、及脂環式環氧化合物,[7]如前述[1]至[6]項中任一項所述之樹脂組合物,更含有光酸產生劑(D),[8]如前述[1]至[7]項中任一項所述之樹脂組合物,其中前述光酸產生劑(D)為醌二疊氮化合物,[9]如前述[1]至[8]項中任一項所述之樹脂組合物,其中前述黏結劑樹脂(A)為具有質子性極性基的環狀烯烴聚合物,[10]如前述[1]至[9]項中任一項所述之樹脂組合物,其中相對於形成前述樹脂組合物之固體成分全體,前述苯氧基樹脂(B)的含有比例為2~75重量%,[11]如前述[1]至[10]項中任一項所述之樹脂組合物,其中前述苯氧基樹脂(B)係具備雙酚結構之苯氧基樹脂,以及[12]一種電子元件,係具備由如前述[1]至[11]項中任一項所述之樹脂組合物所構成之樹脂膜。
依照本發明,能夠提供一種能夠供給具有優異的耐熱性、對基板的密著性、焊料耐熱性、及耐熱衝擊性的樹脂膜之樹脂組合物、及具備由此種樹脂組合物所構成的樹脂膜之電子元件。
本發明的樹脂組合物係含有黏結劑樹脂(A)、羥基當量為300以上的苯氧基樹脂(B)及交聯劑(C)而成。
(黏結劑樹脂(A))
作為在本發明所使用的黏結劑樹脂(A),係沒有特別限定,以具有質子性極性基的環狀烯烴聚合物(A1)、丙烯酸樹脂(A2)、聚醯亞胺或其前驅物(A3)、聚苯並噁唑或其前驅物(A4)、聚矽氧烷(A5)或酚樹脂(A6)為佳,該等之中,以具有質子性極性基的環狀烯烴聚合物(A1)為特佳。
該等黏結劑樹脂(A),係各自可單獨使用,亦可併用2種以上。
作為具有質子性極性基的環狀烯烴聚合物(A1)(以下,簡稱為「環狀烯烴聚合物(A1)」),可舉出1或2個以上的環狀烯烴單體之聚合物、或1或2個以上的環狀烯烴單體和能夠與其共聚合的單體之共聚物。在本發明,作為用以形成環狀烯烴聚合物(A1)之單體,以使用至少具有質子性極性基之環狀烯烴單體(a)為佳。
在此,所謂質子性極性基,係指含有氫原子直接
鍵結在屬於周期表第15族或第16族的原子之基團。屬於周期表第15族或第16族的原子之中,以屬於周期表第15族或第16族的第1或第2周期之原子為佳,較佳為氧原子、氮原子或硫原子,特佳為氧原子。
作為此種質子性極性基之具體例,可舉出羥基、羧基(羥羰基)、磺酸基、磷酸基等具有氧原子的極性基;第一級胺基、第二級胺基、第一級醯胺基、第二級醯胺基(醯亞胺基)等具有氮原子的極性基;硫醇基等具有硫原子的極性基等。該等之中,以具有氧原子者為佳,較佳為羧基。
在本發明,鍵結在具有質子性極性基的環狀烯烴樹脂之質子性極性基的數目係沒有特別限定,又,亦可含有不同種類的質子性極性基。
作為具有質子性極性基的環狀烯烴單體(a)(以下,簡稱為「單體(a)」)之具體例,可舉出2-羥羰基雙環[2.2.1]庚-5-烯、2-甲基-2-羥羰基雙環[2.2.1]庚-5-烯、2-羧甲基-2-羥羰基雙環[2.2.1]庚-5-烯、2-羥羰基-2-甲氧基羰基甲基雙環[2.2.1]庚-5-烯、2-羥羰基-2-乙氧基羰基甲基雙環[2.2.1]庚-5-烯、2-羥羰基-2-丙氧基羰基甲基雙環[2.2.1]庚-5-烯、2-羥羰基-2-丁氧基羰基甲基雙環[2.2.1]庚-5-烯、2-羥羰基-2-戊氧基羰基甲基雙環[2.2,1]庚-5-烯、2-羥羰基-2-己氧基羰基甲基雙環[2.2.1]庚-5-烯、2-羥羰基-2-環己氧基羰基甲基雙環[2.2.1]庚-5-烯、2-羥羰基-2-苯氧基羰基甲基雙環[2.2.1]庚-5-烯、2-羥羰基-2-萘氧基羰基甲基雙環[2.2.1]庚-5-烯、2-羥羰基-2-聯苯氧基羰基甲基雙環[2.2.1]庚-5-烯、2-羥羰基-2-苄氧基羰基甲基
雙環[2.2.1]庚-5-烯、2-羥羰基-2-羥乙氧基羰基甲基雙環[2.2.1]庚-5-烯、2,3-二羥羰基雙環[2.2.1]庚-5-烯、2-羥羰基-3-甲氧基羰基雙環[2.2.1]庚-5-烯、2-羥羰基-3-乙氧基羰基雙環[2.2.1]庚-5-烯、2-羥羰基-3-丙氧基羰基雙環[2.2.1]庚-5-烯、2-羥羰基-3-丁氧基羰基雙環[2.2.1]庚-5-烯、2-羥羰基-3-戊氧基羰基雙環[2.2.1]庚-5-烯、2-羥羰基-3-己氧基羰基雙環[2.2.1]庚-5-烯、2-羥羰基-3-環己氧基羰基雙環[2.2.1]庚-5-烯、2-羥羰基-3-苯氧基羰基雙環[2.2.1]庚-5-烯、2-羥羰基-3-萘氧基羰基雙環[2.2.1]庚-5-烯、2-羥羰基-3-聯苯氧基羰基雙環[2.2.1]庚-5-烯、2-羥羰基-3-苄氧基羰基雙環[2.2.1]庚-5-烯、2-羥羰基-3-羥乙氧基羰基雙環[2.2.1]庚-5-烯、2-羥羰基-3-羥羰基甲基雙環[2.2.1]庚-5-烯、3-甲基-2-羥羰基雙環[2.2.1]庚-5-烯、3-羥甲基-2-羥羰基雙環[2.2.1]庚-5-烯、2-羥羰基三環[5.2.1.02,6]癸-3,8-二烯、4-羥羰基四環[6.2.1.13,6.02,7]十二-9-烯、4-甲基-4-羥羰基四環[6.2.1.13,6.02,7]十二-9-烯、4,5-二羥羰基四環[6.2.1.13,6.02,7]十二-9-烯、4-羧甲基-4-羥羰基四環[6.2.1.13,6.02,7]十二-9-烯、N-(羥羰基甲基)雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(羥羰基乙基)雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(羥羰基戊基)雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(二羥羰基乙基)雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(二羥羰基丙基)雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(羥羰基苯乙基F)雙環[2,2.1]庚-5-烯-2,3-二羧醯亞胺、N-(2-(4-羥苯基)-1-(羥羰基)乙基)雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(羥羰基苯基)雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺等的羧基含有環狀烯烴;2-(4-羥苯基)雙
環[2.2.1]庚-5-烯、2-甲基-2-(4-羥苯基)雙環[2.2.1]庚-5-烯、4-(4-羥苯基)四環[6.2.1.13,6.02,7]十二-9-烯、4-甲基-4-(4-羥苯基)四環[6.2.1.13,6.02,7]十二-9-烯、2-羥基雙環[2.2.1]庚-5-烯、2-羥甲基雙環[2.2.1]庚-5-烯、2-羥乙基雙環[2.2.1]庚-5-烯、2-甲基-2-羥甲基雙環[2.2.1]庚-5-烯、2,3-二羥甲基雙環[2.2.1]庚-5-烯、2-(羥乙氧基羰基)雙環[2.2.1]庚-5-烯、2-甲基-2-(羥乙氧基羰基)雙環[2.2.1]庚-5-烯、2-(1-羥基-1-三氟甲基-2,2,2-三氟乙基)雙環[2.2.1]庚-5-烯、2-(2-羥基-2-三氟甲基-3,3,3-三氟丙基)雙環[2.2.1]庚-5-烯、3-羥基三環[5.2.1.02,6]癸-4,8-二烯、3-羥甲基三環[5.2.1.02,6]癸-4,8-二烯、4-羥基四環[6.2.1.13,6.02,7]十二-9-烯、4-羥甲基四環[6.2.1.13,6.02,7]十二-9-烯、4,5-二羥甲基四環[6.2.1.13,6.02,7]十二-9-烯、4-(羥乙氧基羰基)四環[6.2.1.13,6.02,7]十二-9-烯、4-甲基-4-(羥乙氧基羰基)四環[6.2.1.13,6.02,7]十二-9-烯、N-(羥乙基)雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(羥苯基)雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺等的羥基含有環狀烯烴等。該等之中,從所得到的樹脂膜之密著性變高的觀點而言,以羧基含有環狀烯烴為佳,以4-羥羰基四環[6.2.1.13,6.02,7]十二-9-烯為特佳。該等單體(a),係各自可單獨使用,亦可組合2種以上而使用。
在環狀烯烴聚合物(A1)中,係相對於總單體單元,單體(a)單元的含有比例係以10~90莫耳%為佳,較佳為20~80莫耳%,更佳為30~70莫耳%。藉由使單體(a)單元的含有比例成為上述範圍,環狀烯烴聚合物(A1)在極性溶劑之溶解性成為良好,同時能夠進一步提高所得到的樹脂膜之耐熱性。
又,在本發明所使用的環狀烯烴聚合物(A1),亦可為具有質子性極性基的環狀烯烴單體(a)和能夠與其共聚合的單體(b)共聚合而得到之共聚物。作為此種能夠共聚合的單體,可舉出具有質子性極性基以外的極性基之環狀烯烴單體(b1)、不具有極性基的環狀烯烴單體(b2)及環狀烯烴以外的單體(b3)(以下,簡稱為「單體(b1)」、「單體(b2)」、「單體(b3)」)。
作為具有質子性極性基以外的極性基之環狀烯烴單體(b1),例如可舉出具有N-取代醯亞胺基、酯基、氰基、酸酐基或鹵素原子之環狀烯烴。
作為具有N-取代醯亞胺基之環狀烯烴,例如可舉出下述通式(1)表示之單體。
(上述通式(1)中,R1係表示氫原子或碳數1~16的烷基或芳基。n係表示1或2的整數)。
在上述通式(1)中,R1為碳數1~16的烷基或芳基,作為烷基的具體例,可舉出甲基、乙基、正丙基、正丁基、正戊基、正己基、正庚基、正辛基、正壬基、正癸基、正十一基、正十二基、正十三基、正十四基、正十五基、正十六基等的直鏈烷基;環丙基、環丁基、環戊基、環己基、環庚基、環辛基、環壬基、環癸基、環十一基、環十二基、降莰基、莰基、異莰
基、十氫萘基、三環癸基、金剛烷基等的環狀烷基;2-丙基、2-丁基、2-甲基-1-丙基、2-甲基-2-丙基、I-甲基丁基、2-甲基丁基、1-甲基戊基、1-乙基丁基、2-甲基己基、2-乙基己基、4-甲基庚基、1-甲基壬基、1-甲基十三基、1-甲基十四基等的分枝狀烷基等。又,作為芳基的具體例,可舉出苯基、苄基等。該等之中,因為耐熱性及對極性溶劑的溶解性較優異,以碳數6~14的烷基及芳基為佳,以碳數6~10的烷基及芳基為較佳。碳數為4以下時,對極性溶劑的溶解性較差,碳數為17以上時,耐熱性較差,而且將樹脂膜圖案化時,會有因熱而熔融而使圖案消失之問題。
作為上述通式(1)表示的單體之具體例,可舉出雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-苯基-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-甲基雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-乙基雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-丙基雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-丁基雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-環己基雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-金剛烷基雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-甲基丁基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(2-甲基丁基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-甲基戊基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(2-甲基戊基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-乙基丁基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(2-乙基丁基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-甲基己基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(2-甲基己基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(3-甲基己基)-雙環
[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-丁基戊基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(2-丁基戊基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-甲基庚基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(2-甲基庚基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(3-甲基庚基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(4-甲基庚基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-乙基己基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(2-乙基己基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(3-乙基己基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-丙基戊基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(2-丙基戊基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-甲基辛基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(2-甲基辛基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(3-甲基辛基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(4-甲基辛基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-乙基庚基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(2-乙基庚基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(3-乙基庚基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(4-乙基庚基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-丙基己基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(2-丙基己基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(3-丙基己基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-甲基壬基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(2-基壬基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(3-甲基壬基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(4-甲基壬基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(5-甲基壬基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、
N-(1-乙基辛基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(2-乙基辛基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(3-乙基辛基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(4-乙基辛基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-甲基癸基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-甲基十二基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-甲基十一基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-甲基十二基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-甲基十三基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-甲基十四基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-(1-甲基十五基)-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺、N-苯基-四環[6.2.1.13,6.02,7]十二-9-烯-4,5-二羧醯亞胺、N-(2,4-二丁氧基苯基)-四環[6.2.1.13,6.02,7]十二-9-烯-4,5-二羧醯亞胺等。又,該等係各自可單獨使用,亦可組合2種以上而使用。
又,上述通式(1)表示之單體,係例如能夠藉由對應的胺、與5-降莰烯-2,3-二羧酸酐的醯亞胺化反應來得到。又,所得到的單體,係能夠藉由習知方法將醯亞胺化反應的反應液分離‧精製而效率良好地純化。
作為具有酯基之環狀烯烴,例如可舉出2-乙醯氧基雙環[2.2.1]庚-5-烯、2-乙醯氧基甲基雙環[2.2.1]庚-5-烯、2-甲氧基羰基雙環[2.2.1]庚-5-烯、2-乙氧基羰基雙環[2.2.1]庚-5-烯、2-丙氧基羰基雙環[2.2.1]庚-5-烯、2-丁氧基羰基雙環[2.2.1]庚-5-烯、2-環己氧基羰基雙環[2.2.1]庚-5-烯、2-甲基-2-甲氧基羰基雙環[2.2.1]庚-5-烯、2-甲基-2-乙氧基羰基雙環[2.2.1]庚-5-烯、2-甲基-2-丙氧基羰基雙環[2.2.1]庚-5-烯、2-甲基-2-丁氧基羰基雙
環[2.2.1]庚-5-烯、2-甲基-2-環己氧基羰基雙環[2.2.1]庚-5-烯、2-(2,2,2-三氟乙氧基羰基)雙環[2.2.1]庚-5-烯、2-甲基-2-(2,2,2-三氟乙氧基羰基)雙環[2.2.1]庚-5-烯、2-甲氧基羰基三環[5.2.1.02,6]癸-8-烯、2-乙氧基羰基三環[5.2.1.02,6]癸-8-烯、2-丙氧基羰基三環[5.2.1.02,6]癸-8-烯、4-乙醯氧基四環[6.2.1.13,6.02,7]十二-9-烯、4-甲氧基羰基四環[6.2.1.13,6.02,7]十二-9-烯、4-乙氧基羰基四環[6.2.1.13,6.02,7]十二-9-烯、4-丙氧基羰基四環[6.2.1.13,6.02,7]十二-9-烯、4-丁氧基羰基四環[6.2.1.13,6.02,7]十二-9-烯、4-甲基-4-甲氧基羰基四環[6.2.1.13,6.02,7]十二-9-烯、4-甲基-4-乙氧基羰基四環[6.2.1.13,6.02,7]十二-9-烯、4-甲基-4-丙氧基羰基四環[6.2.1.13,6.02,7]十二-9-烯、4-甲基-4-丁氧基羰基四環[6.2.1.13,6.02,7]十二-9-烯、4-(2,2,2-三氟乙氧基羰基)四環[6.2.1.13,6.02,7]十二-9-烯、4-甲基-4-(2,2,2-三氟乙氧基羰基)四環[6.2.1.13,6.02,7]十二-9-烯等。
作為具有氰基之環狀烯烴,例如可舉出4-氰基四環[6.2.1.13,6.02,7]十二-9-烯、4-甲基-4-氰基四環[6.2.1.13,6.02,7]十二-9-烯、4,5-二氰基四環[6.2.1.13,6.02,7]十二-9-烯、2-氰基雙環[2.2.1]庚-5-烯、2-甲基-2-氰基雙環[2.2.1]庚-5-烯、2,3-二氰基雙環[2.2.1]庚-5-烯等。
作為具有酸酐基之環狀烯烴,例如可舉出四環[6.2.1.13,6.02,7]十二-9-烯-4,5-二羧酸酐、雙環[2.2.1]庚-5-烯-2,3-二羧酸酐、2-羧甲基-2-羥羰基雙環[2.2.1]庚-5-烯酐等。
作為具有鹵素原子之環狀烯烴,例如可舉出2-氯雙環[2.2.1]庚-5-烯、2-氯甲基雙環[2.2.1]庚-5-烯、2-(氯苯基)
雙環[2.2.1]庚-5-烯、4-氯四環[6.2.1.13,6.02,7]十二-9-烯、4-甲基-4-氯四環[6.2.1.13,6.02,7]十二-9-烯等。
該等單體(b1),係各自可單獨使用,亦可組合2種以上而使用。
作為不具有極性基的環狀烯烴單體(b2),可舉出雙環[2.2.1]庚-2-烯(亦稱為「降莰烯」)、5-乙基-雙環[2.2.1]庚-2-烯、5-丁基-雙環[2.2.1]庚-2-烯、5-亞乙基-雙環[2.2.1]庚-2-烯、5-亞甲基-雙環[2.2.1]庚-2-烯、5-乙烯基-雙環[2.2.1]庚-2-烯、三環[5.2.1.02,6]癸-3,8-二烯(慣用名:二環戊二烯)、四環[10.2.1.02,11.04,9]十五-4,6,8,13-四烯、四環[6.2.1.13,6.02,7]十二-4-烯(亦稱為「四環十二烯」)、9-甲基-四環[6.2.1.13,6.02,7]十二-4-烯、9-乙基-四環[6.2.1.13,6.02,7]十二-4-烯、9-亞甲基-四環[6.2.1.13,6.02,7]十二-4-烯、9-亞乙基-四環[6.2.1.13,6.02,7]十二-4-烯、9-乙烯基-四環[6.2.1.13,6.02,7]十二-4-烯、9-丙烯基-四環[6.2.1.13,6.02,7]十二-4-烯、五環[9.2.1.13,9.02,10.04,8]十五-5,12-二烯、環丁烯、環戊烯、環戊二烯、環己烯、環庚烯、環辛烯、環辛二烯、茚、3a,5,6,7a-四氫-4,7-亞甲基-1H-茚、9-苯基-四環[6.2.1.13,6.02,7]十二-4-烯、四環[9.2.1.02,10.03,8]十四-3,5,7,12-四烯、五環[9.2.1.13,9.02,10.04,8]十五-12-烯等。
該等單體(b2),係各自可單獨使用,亦可組合2種以上而使用。
作為環狀烯烴以外的單體(b3)之具體例,可舉出乙烯;丙烯、1-丁烯、1-戊烯、1-己烯、3-甲基-1-丁烯、3-甲基-1-戊烯、3-乙基-1-戊烯、4-甲基-1-戊烯、4-甲基-丁-己烯、4,4-
二甲基-1-己烯、4,4-二甲基-1-戊烯、4-乙基-1-己烯、3-乙基-1-己烯、1-辛烯、1-癸烯、1-十二烯、1-十四烯、1-十六烯、1-十八烯、1-二十烯等碳數2~20的α-烯烴;1,4-己二烯、1,5-己二烯、4-甲基-1,4-己二烯、5-甲基-1,4-己二烯、1,7-辛二烯等的非共軛二烯、及該等的衍生物等。該等之中,以α-烯烴為佳。
該等單體(b3),係各自可單獨使用,亦可組合2種以上而使用。
該等單體(b1)~(b3)之中,從本發明的效果為進一步更顯著之觀點而言,係以具有質子性極性基以外的極性基之環狀烯烴單體(b1)為佳,以具有N-取代醯亞胺基之環狀烯烴為特佳。
在環狀烯烴聚合物(A1)中,相對於總單體單元,能夠共聚合的單體(b)單元之含有比例,以10~90莫耳%為佳,較佳為20~80莫耳%,更佳為30~70莫耳%。藉由使能夠共聚合的單體(b)單元之含有比例成為上述範圍,在使環狀烯烴聚合物(A1)對極性溶劑的溶解性成為良好之同時,能夠進一步提高所得到的樹脂膜之耐熱性。
又,在本發明,亦可藉由利用習知的改性劑而將質子性極性基導入至不具有質子性極性基的環狀烯烴系聚合物,而作為環狀烯烴聚合物(A1)。
不具有質子性極性基的聚合物,係能夠藉由將上述的單體(b1)及(b2)之中至少一種,必要時,可與單體(b3)任意地組合而聚合來得到。
作為用以導入質子性極性基之改性劑,通常能夠
使用在一個分子內具有質子性極性基及反應性的碳-碳不飽和鍵之化合物。
作為此種化合物的具體例,可舉出丙烯酸、甲基丙烯酸、當歸酸、甲基丁烯酸(tiglic acid)、油酸、反油酸(elaidic acid)、芥子酸、十三烷二酸、順丁烯二酸、反丁烯二酸、檸康酸、中康酸、伊康酸、阿托酸、桂皮酸等的不飽和羧酸;烯丙醇、甲基乙烯基甲醇、巴豆醇、甲基烯丙醇、1-苯乙烯-1-醇、2-丙烯-1-醇、3-丁烯-1-醇、3-丁烯-2-醇、3-甲基-3-丁烯-1-醇、3-甲基-2-丁烯-1-醇、2-甲基-3-丁烯-2-醇、2-甲基-3-丁烯-1-醇、4-戊烯-1-醇、4-甲基-4-戊烯-1-醇、2-己烯-1-醇等的不飽和醇等。
使用該等改性劑之聚合物的改性反應,係依照常用的方法即可,通常能夠在自由基產生劑的存在下進行。
又,在本發明所使用的環狀烯烴聚合物(A1),可為使上述單體開環聚合而成之開環聚合物,或者亦可為使上述單體加成聚合而成之加成聚合物,從本發明的效果進一步更顯著之觀點而言,以開環聚合物為佳。
在複分解反應觸媒的存在下,開環聚合物係能夠藉由將具有質子性極性基的環狀烯烴單體(a)及必要時所使用之能夠共聚合的單體(b)進行開環複分解(metathesis)聚合來製造。製造方法例如能夠使用國際公開第2010/110323號的[0039]~[0079]所記載的方法等。
又,在本發明所使用之環狀烯烴聚合物(A1)為開環聚合物時,以進一步進行氫化反應,將在主鏈所含有的碳-碳雙鍵氫化而成為氫化物為佳。環狀烯烴聚合物(A1)為氫化物
時,經氫化的碳-碳雙鍵之比例(氫化率)係通常50%以上,從耐熱性的觀點而言,以70%以上為佳,以90%以上為較佳,以95%以上為更佳。
又,在本發明所使用之丙烯酸樹脂(A2),係沒有特別限定,以將選自具有丙烯醯基的羧酸、具有丙烯醯基的羧酸酐、或含環氧基的丙烯酸酯化合物及含噁丁環基的丙烯酸酯化合物之至少一種作為必要成分之同元聚合物或共聚物為佳。
作為具有丙烯醯基的羧酸之具體例,係可舉出(甲基)丙烯酸[意即丙烯酸及/或甲基丙烯酸。以下,(甲基)丙烯酸甲酯等亦相同]、巴豆酸、順丁烯二酸、反丁烯二酸、檸康酸、中康酸、戊烯二酸、苯二甲酸單-(2-((甲基)丙烯醯氧基)乙基)酯、N-(羧苯基)順丁烯二醯亞胺、N-(羧苯基)(甲基)丙烯醯胺等。
作為具有丙烯醯基的羧酸酐的具體例,可舉出順丁烯二酸酐、檸康酸酐等。
作為含環氧基的丙烯酸酯化合物之具體例,可舉出丙烯酸縮水甘油酯、甲基丙烯酸縮水甘油酯、α-乙基丙烯酸縮水甘油酯、α-正丙基丙烯酸縮水甘油酯、α-正丁基丙烯酸縮水甘油酯、丙烯酸-3,4-環氧丁酯、甲基丙烯酸-3,4-環氧丁酯、丙烯酸-6,7-環氧庚酯、甲基丙烯酸-6,7-環氧庚酯、α-乙基丙烯酸-6,7-環氧庚酯、丙烯酸-3,4-環氧基環己基甲酯、甲基丙烯酸-3,4-環氧基環己基甲酯等。
作為含噁丁環基的丙烯酸酯化合物之具體例,可舉出(甲基)丙烯酸(3-甲基噁丁環-3-基)甲酯、(甲基)丙烯酸(3-乙基噁丁環-3-基)甲酯、(甲基)丙烯酸(3-甲基噁丁環-3-基)乙酯、(甲基)
丙烯酸(3-乙基噁丁環-3-基)乙酯、(甲基)丙烯酸(3-氯甲基噁丁環-3-基)甲酯、(甲基)丙烯酸(噁丁環-2-基)甲酯、(甲基)丙烯酸(2-甲基噁丁環--2-基)甲酯、(甲基)丙烯酸(2-乙基噁丁環-2-基)甲酯、(1-甲基-1-噁丁環基-2-苯基)-3-(甲基)丙烯酸酯、(1-甲基-1-噁丁環基)-2-三氟甲基-3-(甲基)丙烯酸酯、及(1-甲基-1-噁丁環基)-4-三氟甲基-2-(甲基)丙烯酸酯等。
該等之中,以(甲基)丙烯酸、順丁烯二酸酐、(甲基)丙烯酸縮水甘油酯、甲基丙烯酸-6,7-環氧庚酯等為佳。
丙烯酸樹脂(A2)亦可為選自不飽和羧酸、不飽和羧酸酐及含環氧基的不飽和化合物之至少一種、與其它的丙烯酸酯系單體或丙烯酸酯以外之能夠共聚合的單體之共聚物。
作為其它的丙烯酸酯系單體,可舉出(甲基)丙烯酸甲酯、(甲基)丙烯酸乙酯、(甲基)丙烯酸丙酯、(甲基)丙烯酸異丙酯、(甲基)丙烯酸丁酯、(甲基)丙烯酸異丁酯、(甲基)丙烯酸第三丁酯、(甲基)丙烯酸戊酯、(甲基)丙烯酸異戊酯、(甲基)丙烯酸己酯、(甲基)丙烯酸庚酯、(甲基)丙烯酸辛酯、(甲基)丙烯酸異辛酯、(甲基)丙烯酸乙基己酯、(甲基)丙烯酸壬酯、(甲基)丙烯酸癸酯、(甲基)丙烯酸異癸酯、(甲基)丙烯酸十一酯、(甲基)丙烯酸十二酯、(甲基)丙烯酸月桂酸酯、(甲基)丙烯酸硬脂酸酯、(甲基)丙烯酸異硬脂酸酯等的(甲基)丙烯酸烷酯;(甲基)丙烯酸羥基乙酯、(甲基)丙烯酸2-羥基丙酯、(甲基)丙烯酸3-羥基丙酯、(甲基)丙烯酸2-羥基丁酯、(甲基)丙烯酸3-羥基丁酯、(甲基)丙烯酸4-羥基丁酯等的(甲基)丙烯酸羥基烷酯;(甲基)丙烯酸苯氧基乙酯、(甲基)丙烯酸2-羥基-3-苯氧基丙酯
等的(甲基)丙烯酸苯氧基烷酯;(甲基)丙烯酸2-甲氧基乙酯、(甲基)丙烯酸2-乙氧基乙酯、(甲基)丙烯酸2-丙氧基乙酯、(甲基)丙烯酸2-丁氧基乙酯、(甲基)丙烯酸2-甲氧基丁酯等的(甲基)丙烯酸烷氧基烷酯;聚乙二醇一(甲基)丙烯酸酯、乙氧基二乙二醇(甲基)丙烯酸酯、甲氧基聚乙二醇(甲基)丙烯酸酯、苯氧基聚乙二醇(甲基)丙烯酸酯、壬基苯氧基聚乙二醇(甲基)丙烯酸酯、聚丙二醇一(甲基)丙烯酸酯、甲氧基聚丙二醇(甲基)丙烯酸酯、乙氧基聚丙二醇(甲基)丙烯酸酯、壬基苯氧基聚丙二醇(甲基)丙烯酸酯等的聚烷二醇(甲基)丙烯酸酯;(甲基)丙烯酸環己酯、(甲基)丙烯酸2-甲基環己酯、(甲基)丙烯酸4-丁基環己酯、(甲基)丙烯酸1-金剛烷酯、(甲基)丙烯酸2-甲基-2-金剛烷酯、(甲基)丙烯酸2-乙基-2-金剛烷酯、(甲基)丙烯酸三環[5.2.1.02,6]癸烷-8-基酯、(甲基)丙烯酸三環[5.2.1.02,6]-3-癸烯-8-基酯、(甲基)丙烯酸三環[5.2.1.02,6]-3-癸烯-9-基酯、(甲基)丙烯酸莰酯、(甲基)丙烯酸異莰酯等的(甲基)丙烯酸環烷酯;(甲基)丙烯酸苯酯、(甲基)丙烯酸萘酯、(甲基)丙烯酸聯苯酯、(甲基)丙烯酸苄酯、(甲基)丙烯酸四氫糠酯、(甲基)丙烯酸5-四氫糠氧基羰基戊酯、(甲基)丙烯酸乙烯酯、(甲基)丙烯酸烯丙酯、(甲基)丙烯酸2-(2-乙烯氧基乙氧基)乙酯、(甲基)丙烯酸2-[三環[5.2.1.02,6]癸烷-8-基氧基]乙酯、(甲基)丙烯酸2-[三環[5.2.1.02,6]-3-癸烯-8-基氧基]乙酯、(甲基)丙烯酸2-[三環[5.2.1.02,6]-3-癸烯-9-基氧基]乙酯、(甲基)丙烯酸γ-丁內酯、順丁烯二醯亞胺、N-甲基順丁烯二醯亞胺、N-乙基順丁烯二醯亞胺、N-丁基順丁烯二醯亞胺、N-環己基順丁烯二醯亞胺、N-
苄基順丁烯二醯亞胺、N-苯基順丁烯二醯亞胺、N-(2,6-二乙基苯基)順丁烯二醯亞胺、N-(4-乙醯基苯基)順丁烯二醯亞胺、N-(4-羥苯基)順丁烯二醯亞胺、N-(4-乙醯氧基苯基)順丁烯二醯亞胺、N-(4-二甲胺基-3,5-二硝基苯基)順丁烯二醯亞胺、N-(1-苯胺基萘基-4)順丁烯二醯亞胺、N-[4-(2-苯並噁唑基)苯基]順丁烯二醯亞胺、N-(9-吖啶基)順丁烯二醯亞胺等。
該等之中,以(甲基)丙烯酸甲酯、(甲基)丙烯酸丁酯、(甲基)丙烯酸環己酯、(甲基)丙烯酸2-甲基環己酯、(甲基)丙烯酸苄酯、(甲基)丙烯酸三環[5.2.1.02,6]癸烷-8-基酯、N-苯基順丁烯二醯亞胺及N-環己基順丁烯二醯亞胺等為佳。
作為丙烯酸酯以外之能夠共聚合的單體,只要是上述能夠與具有丙烯醯基的羧酸、具有丙烯醯基的羧酸酐或含環氧基的丙烯酸酯化合物共聚合的化合物,就沒有特別限制,例如可舉出乙烯基苄基甲醚、乙烯基環氧丙基醚、苯乙烯、α-甲基苯乙烯、乙烯基甲苯、茚、乙烯基萘、乙烯基聯苯、氯苯乙烯、溴苯乙烯、氯甲基苯乙烯、對第三丁氧基苯乙烯、對羥基苯乙烯、對羥基-α-甲基苯乙烯、對乙醯氧基苯乙烯、對羧基苯乙烯、4-羥苯基乙烯基酮、丙烯腈、甲基丙烯腈、(甲基)丙烯醯胺、1,2-環氧基-4-乙烯基環己烷、異丁烯、降莰烯、丁二烯、異戊二烯等的自由基聚合性化合物。
該等化合物,係各自可單獨使用,亦可組合2種以上而使用。
上述單體的聚合方法,係依照常用的方法即可,例如能夠採用懸浮聚合法、乳化聚合法、溶液聚合法等。
在本發明所使用之聚醯亞胺、或其前驅物(A3),係能夠藉由使四羧酸二酐與二胺反應而得到,必要時,可進行熱處理。作為用以得到聚醯亞胺之前驅物,可舉出聚醯胺酸、聚醯胺酸酯、聚異醯亞胺、聚醯胺酸磺醯胺等。
在本發明所使用之聚醯亞胺、或其前驅物(A3)係能夠使用習知的方法合成。亦即,能夠使用將四羧酸二酐與二胺選擇性地組合,使該等在N-甲基-2-吡咯啶酮、N,N-二甲基乙醯胺、N,N-二甲基甲醯胺、二甲基亞碸、六甲基磷醯三胺、γ-丁內酯、環戊酮等的極性溶劑中反應等習知的方法來合成。
使二胺超量而聚合時,能夠使所生成的聚醯亞胺(A3)之末端胺基與羧酸酐反應,而保護末端胺基。又,使四羧酸二酐超量而聚合時,亦能夠使所生成的聚醯亞胺(A3)之末端酸酐基與胺化合物反應,而保護末端酸酐基。
作為此種羧酸酐的例子,能夠舉出苯二甲酸酐、偏苯三甲酸酐、順丁烯二酸酐、萘二甲酸酐、氫化苯二甲酸酐、甲基-5-降莰烯-2,3-二羧酸酐、伊康酸酐、四氫苯二甲酸酐等;作為胺化合物的例子,能夠舉出苯胺、2-羥基苯胺、3-羥基苯胺、4-羥基苯胺、2-乙炔基苯胺、3-乙炔基苯胺、4-乙炔基苯胺等。
聚苯並噁唑、或其前驅物(A4),係能夠藉由使雙(鄰胺基苯酚)化合物與二羧酸、二羧酸酯、羧醯二氯反應而得到,必要時,亦可進行加熱處理。
作為在本發明所使用之聚矽氧烷(A5),係沒有特別限定,可舉出較佳是藉由使下述通式(2)表示的有機矽烷之1
種或2種以上混合、反應而得到之聚合物。
(R2)p-Si-(OR3)4-p (2)
上述通式(2)中,R2為氫原子、碳數1~10的烷基、碳數2~10的烯基、或碳數6~15的芳基,複數個R2係各自可相同亦可不同。又,該等烷基、烯基、芳基係任一者均亦可具有取代基,又,亦可為不具有取代基的未取代物,能夠按照組合物的特性而選擇。作為烷基的具體例,可舉出甲基、乙基、正丙基、異丙基、正丁基、第三丁基、正己基、正癸基、三氟甲基、2,2,2-三氟乙基、3,3,3-三氟丙基、3-環氧丙基丙基、2-(3,4-環氧基環己基)乙基、3-胺丙基、3-氫硫基丙基、3-異氰酸酯丙基。作為烯基的具體例,可舉出乙烯基、3-丙烯醯氧基丙基、3-甲基丙烯醯氧基丙基。作為芳基的具體例,可舉出苯基、甲苯基、對羥基苯基、1-(對羥苯基)乙基、2-(對羥苯基)乙基、4-羥基-5-(對羥苯基羰氧基)戊基、萘基。
又,上述通式(2)中,R3係氫原子、碳數1~6的烷基、碳數1~6的醯基、或碳數6~15的芳基,複數個R3係各自可相同亦可不同。又,該等烷基、醯基係任一者均亦可具有取代基,又,亦可為不具有取代基的未取代物,能夠按照組合物的特性而選擇。作為烷基的具體例,可舉出甲基、乙基、正丙基、異丙基、正丁基。作為醯基的具體例,可舉出乙醯基。作為芳基的具體例,可舉出苯基。
而且,上述通式(2)中,p為0~3的整數,p=0時,為4官能性矽烷,p=1時,為3官能性矽烷、p=2時,為2官能性矽烷,p=3時,係成為1官能性矽烷。
作為上述通式(2)表示的有機矽烷之具體例,可舉出四甲氧基矽烷、四乙氧基矽烷、四乙醯氧基矽烷、四苯氧基矽烷等的4官能性矽烷;甲基三甲氧基矽烷、甲基三乙氧基矽烷、甲基三異丙氧基矽烷、甲基三正丁氧基矽烷、乙基三甲氧基矽烷、乙基三乙氧基矽烷、乙基三異丙氧基矽烷、乙基三正丁氧基矽烷、正丙基三甲氧基矽烷、正丙基三乙氧基矽烷、正丁基三甲氧基矽烷、正丁基三乙氧基矽烷、正己基三甲氧基矽烷、正己基三乙氧基矽烷、癸基三甲氧基矽烷、乙烯基三甲氧基矽烷、乙烯基三乙氧基矽烷、3-甲基丙烯醯氧基丙基三甲氧基矽烷、3-甲基丙烯醯氧基丙基三乙氧基矽烷、3-丙烯醯氧基丙基三甲氧基矽烷、苯基三甲氧基矽烷、苯基三乙氧基矽烷、對羥苯基三甲氧基矽烷、1-(對羥苯基)乙基三甲氧基矽烷、2-(對羥苯基)乙基三甲氧基矽烷、4-羥基-5-(對羥苯基羰氧基)戊基三甲氧基矽烷、三氟甲基三甲氧基矽烷、三氟甲基三乙氧基矽烷、3,3,3-三氟丙基三甲氧基矽烷、3-胺丙基三甲氧基矽烷、3-胺丙基三乙氧基矽烷、3-環氧丙氧基丙基三甲氧基矽烷、2-(3,4-環氧環己基)乙基三甲氧基矽烷、3-氫硫基丙基三甲氧基矽烷等的3官能性矽烷;二甲基二甲氧基矽烷、二甲基二乙氧基矽烷、二甲基二乙醯氧基矽烷、二正丁基二甲氧基矽烷、二苯基二甲氧基矽烷等的2官能性矽烷;三甲基甲氧基矽烷、三正丁基乙氧基矽烷等的1官能性矽烷。
該等有機矽烷之中,就所得到的樹脂膜之耐龜裂性和硬度而言,使用3官能性矽烷較佳。該等有機矽烷係可單獨使用,亦可以組合2種以上而使用。
在本發明所使用之聚矽氧烷(A5),係能夠藉由使上述的有機矽烷水解及部分縮合來得到。水解及部分縮合係能夠使用通常的方法。例如將溶劑、水、及必要時,將觸媒添加在混合物且加熱攪拌。攪拌中,必要時,亦可藉由蒸餾而將水解副產物(甲醇等的醇類)和縮合副產物(水)餾去。
作為在本發明所使用之酚樹脂(A6),例如能夠藉由在酸觸媒存在下,使酚化合物與醛、二羥甲基化合物、二烷氧基甲基化合物、二鹵甲基化合物反應來得到。
在本發明所使用的黏結劑樹脂(A)之重量平均分子量(Mw),係通常為1,000~1,000,000,以1,500~100,000為佳,較佳為2,000~30,000的範圍。
又,黏結劑樹脂(A)的分子量分布,係以重量平均分子量/數量平均分子量(Mw/Mn)之比,通常為4以下,以3以下為佳,較佳為2.5以下。
黏結劑樹脂(A)的重量平均分子量(Mw)和分子量分布(Mw/Mn),係能夠藉由以四氫呋喃等溶劑作為溶離液之凝膠滲透層析法(GPC),且以聚苯乙烯換算值的方式所求取之值。
(羥基當量為300以上之苯氧基樹脂(B))
本發明的樹脂組合物係除了黏結劑樹脂(A)以外,亦含有羥基當量為300以上之苯氧基樹脂(B)(以下,簡稱為「苯氧基樹脂(B)」)。藉由混合羥基當量為300以上之苯氧基樹脂(B),能夠使耐熱性及焊料耐熱性成為良好,同時提升樹脂膜的伸長度,藉此,能夠使所得到的樹脂膜,成為具有優異的耐熱衝擊性者。又,藉由能夠使樹脂膜的伸長度提升,能夠使所得到的
樹脂膜之可撓性提升,且抑制樹脂膜與基板界面的應力集中,而且能夠使所得到的樹脂膜之對基板的密著性成為優異者。
作為在本發明所使用的苯氧基樹脂(B),羥基當量(g/eq.)為300以上即可,以羥基當量為303以上者為佳,以羥基當量為310以上者為較佳。羥基當量太低時,所得到的樹脂膜係成為耐熱性及焊料耐熱性較差者。又,羥基當量的上限係沒有特別限定,以1000以下為佳,較佳為900以下。
作為苯氧基樹脂(B),例如可舉出具有選自雙酚A骨架、雙酚F骨架、雙酚S骨架、雙酚苯乙酮骨架、酚醛骨架、聯苯基骨架、芴骨架、二環戊二烯骨架、降莰烯骨架、萘骨架、蒽骨架、金剛烷骨架、萜烯骨架、三甲基環己烷骨架之1種以上的骨架者。該等之中,從能夠使本發明的作用效果變得更顯著之觀點而言,係以雙酚A骨架、雙酚F骨架、雙酚S骨架、雙酚苯乙酮骨架等具備雙酚結構者為較佳。
在本發明所使用的苯氧基樹脂(B)之重量平均分子量係沒有特別限定,以5,000~200,000為佳,較佳為10,000~150,000,更佳為15,000~100,000。重量平均分子量為上述範圍時,能夠進一步提高苯氧基樹脂(B)的添加效果。
在本發明的樹脂組合物中,相對於形成本發明的樹脂組合物之固體成分全體100重量%(亦即,在將溶劑等的揮發成分除去後所含有的成分100重量%),苯氧基樹脂(B)的含量係以2~75重量%為佳,較佳為3~70重量%,更佳為4~65重量%,又更佳為6~30重量%,特佳為10~25重量%。相對於形成本發明的樹脂組合物之固體成分全體100重量%,苯氧基樹
脂(B)的含量太少時,有無法得到對基板的密著性及耐熱衝擊性的提升效果之情形,另一方面,太多時,有耐熱性及焊料耐熱性低落之情形。又,相對於形成本發明的樹脂組合物之固體成分全體,苯氧基樹脂(B)的含量係成為上述範圍即可,但是相對於黏結劑樹脂(A)100重量份,苯氧基樹脂(B)的含量係以2~350重量份為佳,較佳為3~325重量份,更佳為4~300重量份,又更佳為10~45重量份,特佳為15~40重量份。
(交聯劑(C))
本發明的樹脂組合物,係除了黏結劑樹脂(A)及苯氧基樹脂(B)以外,亦含有交聯劑(C)。作為交聯劑(C),係藉由加熱而在交聯劑分子間形成交聯結構者;或與黏結劑樹脂(A)反應而在樹脂分子間形成交聯結構者;具體而言,可舉出具有2個以上的反應性基之化合物。作為具有此種反應性基的化合物係沒有特別限定,例如可舉出含環氧基交聯劑、含噁丁環基交聯劑、含異氰酸酯基交聯劑、含嵌段異氰酸酯基交聯劑、含噁唑啉基交聯劑、含順丁烯二醯亞胺基交聯劑、含(甲基)丙烯酸酯基交聯劑、在分子內含有2個以上的烷氧基甲基或羥甲基之化合物等。該等之中,係以含環氧基交聯劑、和在分子內含有2個以上的烷氧基甲基或羥甲基之化合物為佳,從能夠使本發明的作用效果更顯著者之觀點而言,係以將含環氧基交聯劑、及在分子內具有2個以上的烷氧基甲基或羥甲基之化合物併用為較佳。
作為含環氧基交聯劑的具體例,例如可舉出以二環戊二烯作為骨架之環氧化合物(商品名「HP-7200」、DIC公司製)、2,2-雙(羥甲基)1-丁醇的1,2-環氧基-4-(2-環氧乙基)環
己烷加成物(具有環己烷骨架及末端環氧基之15官能性的脂環式環氧樹脂、商品名「EHPE3150」、Daicel化學工業公司製)、環氧化3-環己烯-1,2-二羧酸雙(3-環己烯基甲基)改性ε-己內酯(脂肪族環狀3官能性的環氧樹脂、商品名「EPOLEAD GT301」、Daicel化學工業公司製)、環氧化丁烷四羧酸肆(3-環己烯基甲基)改性ε-己內酯(脂肪族環狀4官能性的環氧樹脂、商品名「EPOLEAD GT401」、Daicel化學工業公司製)、3,4-環氧基環己烯基甲基-3’,4’-環氧基環己烯羧酸酯(商品名「CELLOXIDE 2021」、「CELLOXIDE 2021P」、Daicel化學工業公司製)、ε-己內酯改性3’,4’-環氧基環己基甲基-3,4-環氧基環己烷羧酸酯(商品名「CELLOXIDE 2081」、Daicel化學工業公司製)、1,2:8,9-二環氧薴烯(商品名「CELLOXIDE 3000」、Daicel化學工業公司製)、2-(3,4-環氧基環己基)乙基三甲氧基矽烷(商品名「Z-6043」、TORAY‧DOW CORNING公司製)等具有脂環結構的環氧化合物;
雙酚A型環氧化合物(商品名「jER 825」、「jER 827」、「jER 828」、「jER YL980」、三菱化學公司製、商品名「EPICLON 840」、「EPICLON 850」、DIC公司製)、雙酚F型環氧化合物(商品名「jER 806」、「jER 807」、「jER YL983U」、三菱化學公司製、商品名「EPICLON 830」、「EPICLON 835」、DIC公司製)、氫化雙酚A型環氧化合物(商品名「jER YX8000」、「jER YX8034」三菱化學公司製、商品名「ST-3000」新日鐵柱公司製、商品名「RIKARESIN HBE-100」新日本理化公司製、商品名「Epolite 4000」共榮化學公司製)、長鏈雙酚A
型環氧樹脂(商品名「EXA-4816」、「EXA-4850-150」、「EXA-4850-1000」DIC公司製)、EO改性雙酚A型環氧化合物(商品名「ADEKARESIN EP-4000L」、「ADEKARESIN EP-4010L」、ADEKA公司製)、苯酚酚醛型多官能環氧化合物(商品名「jER 152」、三菱化學公司製)、1,6-雙(2,3-環氧基丙烷-1-基氧基)萘等具有萘骨架的多官能環氧化合物(商品名「HP-4032D」、DIC公司製)、二環戊二烯二甲醇二環氧丙基醚(商品名「ADEKARESIN EP-4000L」、「ADEKARESIN EP-4088L」、ADEKA公司製)、環氧丙基胺型環氧樹脂(商品名「商品名「jER 630」、三菱化學公司製、商品名「TETRAD-C」、「TETRAD-X」、三菱氣體化學公司製)、鏈狀烷基多官能環氧化合物(商品名「SR-TMP」、阪本藥品工業公司製)、多官能環氧聚丁二烯(商品名「EPOLEAD PB3600」、Daicel化學工業公司製)、(商品名「EPOLEAD PB4700」、Daicel化學工業公司製)、甘油的環氧丙基聚醚化合物(商品名「SR-GLG」、阪本藥品工業公司製)、二甘油聚環氧丙基醚化合物(商品名「SR-DGE」、阪本藥品工業公司製、聚甘油聚環氧丙基醚化合物(商品名「SR-4GL」、阪本藥品工業公司製)、γ-環氧丙基丙基三甲基矽烷(商品名「Z6040」、TORAY‧DOW CORNING公司製)等不具有脂環結構的環氧化合物等。
該等含環氧基交聯劑之中,係以具有脂環結構的環氧化合物、亦即脂環式環氧化合物為佳。
作為在分子內含有2個以上的烷氧基甲基之化合物,只要具有2個以上的烷氧基甲基之化合物,就沒有特別限
定,作為2個以上的烷氧基甲基直接鍵結在芳香環而成之酚化合物,例如可舉出2,6-二甲氧基甲基-4-第三丁基苯酚、2,6-二甲氧基甲基-對甲酚等的二甲氧基甲基取代酚化合物、3,3’,5,5’-四甲氧基甲基-4,4’-二羥基聯苯基(例如、商品名「TMOM-BP」、本州化學工業公司製)、1,1-雙[3,5-二(甲氧基甲基)-4-羥苯基]-1-苯基乙烷等的四甲氧基甲基取代聯苯基化合物、4,4’,4”-(亞乙基)參苯酚等的六甲氧基甲基取代化合物(例如、商品名「HMOM-TPHAP-GB」、本州化學工業公司製)等的六甲氧基甲基取代三苯基化合物等。
作為在分子內含有2個以上的羥甲基之化合物,只要是含有2個以上的羥甲基之化合物,就沒有特別限定,係為2個以上的羥甲基直接鍵結在芳香環而成之酚化合物,可舉出2,4-2,4-二羥甲基-6-甲基苯酚、2,6-雙(羥甲基)-對甲酚、4-第三-2,6-雙(羥甲基)苯酚、雙(2-羥基-3-羥甲基-5-甲基苯基)甲烷(商品名「DM-BIPC-F」、旭有機材公司製)、雙(4-羥基-3-羥甲基-5-甲基苯基)甲烷(商品名「DM-BIOC-F」、旭有機材公司製)、2,2-雙(4-羥基-3,5-二羥甲基苯基)丙烷(商品名「TM-BIP-A」、旭有機材公司製)等。
作為在分子內含有2個以上的烷氧基甲基之化合物,就胺基被2個以上的烷氧基甲基取代而成之三聚氰胺化合物而言,例如可舉出N,N’-二甲氧基甲基三聚氰胺、N,N’,N”-三甲氧基甲基三聚氰胺、N,N,N’,N”-四甲氧基甲基三聚氰胺、N,N,N’,N’,N”-五甲氧基甲基三聚氰胺、N,N,N’,N’,N”,N”-六甲氧基甲基三聚氰胺(例如、「Nikalac MW-390LM」「NikalacMW-100LM」、三和Chemical
公司製)、或該等的聚合物等。
作為在分子內含有2個以上的烷氧基甲基之化合物,就被2個以上的烷氧基甲基取代而成之脲化合物而言,可舉出「Nikalac MX270」、三和Chemical公司製,「Nikalac MX280」、三和Chemical公司製,Nikalac MX290」、三和Chemical公司製等。
在分子內含有2個以上的烷氧基甲基、或羥甲基之化合物,係各自能夠單獨、或組合2種以上而使用。
該等之中,從反應性較高的觀點而言,以N,N,N’,N’,N”,N”-六甲氧基甲基三聚氰胺為佳。
交聯劑(C)的分子量係沒有特別限定,通常50~100,000,以80~10,000為佳,較佳為100~5,000。交聯劑(C)係各自可單獨或組合2種以上而使用。
在本發明的樹脂組合物中之交聯劑(C)的含量,係相對於黏結劑樹脂(A)100重量份,以1~80重量份為佳,較佳為5~75重量份,更佳為10~70重量份。藉由使交聯劑(C)的含量成為該範圍,能夠更適當地提高使用本發明的樹脂組合物而得到的樹脂膜之耐熱性。又,作為交聯劑(C),係使用2種以上的化合物時,使合計含量成為上述範圍即可。
(光酸產生劑(D))
又,本發明的樹脂組合物,係除了黏結劑樹脂(A)、苯氧基樹脂(B)及交聯劑(C)以外,亦可進一步含有光酸產生劑(D)。藉由含有光酸產生劑(D),能夠藉由照射紫外線、電子射線等的放射線,使光酸產生劑(D)引起學反應而使由樹脂組合物所
形成的樹脂膜之鹼溶解性產生變化,藉此,能夠使所得到的樹脂膜成為可圖案化者。
作為光酸產生劑(D),例如可舉出苯乙酮化合物、三芳基鋶鹽、醌二疊氮化合物等的疊氮化合物等,較佳為疊氮化合物,特佳為醌二疊氮化合物。
作為醌二疊氮化合物,例如能夠使用醌二疊氮磺醯鹵與具有酚性羥基的化合物之酯化合物。作為醌二疊氮磺醯鹵的具體例,可舉出1,2-萘醌二疊氮-5-磺醯氯、1,2-萘醌二疊氮-4-磺醯氯、1,2-苯醌二疊氮-5-磺醯氯等。作為具酚性羥基的化合物之代表例,可舉出1,1,3-參(2,5-二甲基-4-羥苯基)-3-苯基丙烷、4,4’-[1-[4-[1-[4-羥苯基]-1-甲基乙基]苯基]亞乙基]雙酚等。作為具有該等以外的酚性羥基之化合物,可舉出2,3,4-三羥基二苯基酮、2,3,4,4’-四羥基二苯基酮、2-雙(4-羥苯基)丙烷、參(4-羥苯基)甲烷、1,1,1-參(4-羥基-3-甲基苯基)乙烷、1,1,2,2-肆(4-羥苯基)乙烷、酚醛樹脂的寡聚物、具有1個以上的酚性羥基之化合物與二環戊二烯共聚合而得到之寡聚物等。
又,作為光酸產生劑(D),係除了醌二疊氮化合物以外,亦能夠使用鎓鹽、鹵化有機化合物、α,α’-雙(磺醯基)重氮甲烷系化合物、α-羰基-α’-磺醯基重氮甲烷系化合物、碸化合物、有機酸酯化合物、有機酸醯胺化合物、有機酸醯亞胺化合物等的習知物。
該等光酸產生劑(D)係各自能夠單獨、或組合2種以上而使用。
相對於黏結劑樹脂(A)100重量份,在本發明的樹脂
組合物中之光酸產生劑(D)的含量,係以5~100重量份為佳,較佳為10~60重量份,更佳為15~40重量份。因為在圖案化由樹脂組合物所構成的樹脂膜時,放射線照射部與放射線未照射部對顯影液的溶解度差變大,且放射線敏感度亦變高,容易藉由顯影而圖案化,所以光酸產生劑(D)的含量為上述範圍是適合的。
(其它混合劑)
又,本發明的樹脂組合物亦可進一步含有溶劑。作為溶劑,係沒有特別限定,可舉出習知作為樹脂組合物的溶劑者,例如丙酮、甲基乙基酮、環戊酮、2-己酮、3-己酮、2-庚酮、3-庚酮、4-庚酮、2-辛酮、3-辛酮、4-辛酮等的直鏈的酮類;正丙基醇、異丙醇、正丁醇、環己醇等的醇類;乙二醇二甲醚、乙二醇二乙基醚、二噁烷等的醚類;乙二醇一甲醚、乙二醇一乙醚等的醇類醚類;甲酸丙酯、甲酸丁酯、乙酸丙酯、乙酸丁酯、丙酸甲酯、丙酸乙酯、酪酸甲酯、酪酸乙酯、乳酸甲酯、乳酸乙酯等的酯類;賽路蘇乙酸酯、甲基賽路蘇乙酸酯、乙基賽路蘇乙酸酯、丙基賽路蘇乙酸酯、丁基賽路蘇乙酸酯等的賽路蘇酯類;丙二醇、丙二醇一甲醚、丙二醇一甲醚乙酸酯、丙二醇一乙醚乙酸酯、丙二醇一丁醚等的丙二醇類;二乙二醇一甲醚、二乙二醇一乙醚、二乙二醇二甲醚、二乙二醇二乙醚、二乙二醇甲基乙基醚等的二乙二醇類;γ-丁內酯、γ-戊內酯、γ-己內酯、γ-辛內酯等的飽和γ-內酯類;三氯乙烯等的鹵化烴類;甲苯、二甲苯等的芳香族烴顏;二甲基乙醯胺、二甲基甲醯胺、N-甲基乙醯胺等的極性溶劑等。該等溶劑係可單獨亦可組合2種以上而使用。溶劑的含量係相對於黏結劑樹脂(A)100
重量份,以10~10000重量份為佳,較佳為50~5000重量份,更佳為100~1000重量份的範圍。又,使樹脂組合物含有溶劑時,溶劑係通常在樹脂膜形成之後被除去。
又,本發明的樹脂組合物係只要在不阻礙本發明的效果之範圍內,可依照需要而含有具有酸性基或熱潛在性酸性基的化合物、界面活性劑、敏化劑、光安定劑、消泡劑、顏料、染料、填料等其它混合劑等。該等之中,例如具有酸性基或熱潛在性酸性基之化合物,亦能夠使用在特開2014-29766號公報所記載者等,又,界面活性劑、敏化劑、光安定劑係能夠使用在特開2011-75609號公報所記載者等。但是,該等其它混合劑之中,從樹脂組合物的流動性低落且接著性變差的觀點而言,相對於形成本發明的樹脂組合物之固體成分全體100重量%,填料的混合量係以設為80重量%以下為佳。而且,從減低塗佈本發明的樹脂組合物時之不均的觀點而言,填料的混合量係以設為0重量%為較佳。亦即,以實質上不含有填料(特別是無機填料)為較佳。又,作為填料,係對本發明所使用的黏結劑樹脂(A)不顯示溶解性,而且由於藉由通常的外力時其形狀不產生變化而具有作為填充劑的作用者即可,其形狀可為粒狀、鱗片狀、纖維狀等任一形狀。作為填料,例如可舉出聚醯亞胺粒子、氧化矽、碳黑等的無機填料、以及橡膠粒子等的有機填料等。
本發明的樹脂組合物之調製方法係沒有特別限定,使用習知的方法將構成樹脂組合物之各成分進行混合即可。
混合方法係沒有特別限定,以將使構成樹脂組合物的各成
分溶解或分散在溶劑而得到的溶液或分散液進行混合為佳。藉此,能夠以溶液或分散液的形態得到樹脂組合物。
使構成樹脂組合物的各成分溶解或分散在溶劑之方法,係依照常用的方法即可。具體而言,能夠是使用攪拌子及磁力攪拌器之攪拌;及使用高速均化器、分散器、行星攪拌機、雙軸攪拌機、球磨機、三輥磨機等而進行。又,使各成分溶解或分散在溶劑之後,例如亦可使用孔徑為0.5μm左右的過濾器等進行過濾。
本發明的樹脂組合物之固體成分濃度係通常1~70重量%,以5~60重量%為佳,較佳為10~50重量%。固體成分濃度為該範圍時,溶解安定性、塗佈性和所形成的樹脂膜之膜厚均勻性、平坦性等能夠高度地得到平衡。
(電子元件)
本發明的電子元件,係具有由上述本發明的樹脂組合物所構成的樹脂膜。
作為本發明的電子元件係沒有特別限定,因為由本發明樹脂組合物所構成的樹脂膜係具有優異的耐熱性、對基板的密著性、焊料耐熱性、及耐熱衝擊性,以使用晶圓等級封裝技術所製造之電子元件為佳,特別是由本發明的樹脂組合物所構成之樹脂膜,在使用晶圓等級封裝技術所製造的電子元件,以使用作為形成層間絕緣膜,用以將配置成為層狀之配線之間進行絕緣為較佳。
在本發明的電子元件,作為形成樹脂膜之方法,係沒有特別限定,例如能夠使用塗佈法、薄膜層積法等的方法。
塗佈法,係例如將樹脂組合物塗佈之後,進行加熱乾燥而除去溶劑之方法。作為塗佈樹脂組合物之方法,例如能夠採用噴霧法、旋轉塗佈法、輥塗佈法、模塗佈法、刮刀片法、旋轉塗佈法、棒塗佈法、網版印刷法、噴墨法等的各種方法。加熱乾燥條件係按照各成分的種類和混合比例而不同,通常為30~150℃,以60~120℃為佳,通常為0.5~90分鐘,以1~60分鐘為佳,較佳是進行1~30分鐘即可。
薄膜層積法,係將樹脂組合物塗佈在樹脂薄膜、金屬薄膜等的B階薄膜形成用基材上之後,藉由加熱乾燥將溶劑除去而得到B階薄膜,其次,係層積B階薄膜之方法。加熱乾燥條件係能夠按照各成分的種類和混合比例而適當地選擇,加熱溫度係通常30~150℃,加熱時間係通常0.5~90分鐘。薄膜層積係能夠使用加壓貼合機、衝壓機、真空貼合機、真空衝壓機、輥貼合機等的壓黏機而進行。
作為樹脂膜的厚度係沒有特別限定,按照用途而適當地設定即可,以0.1~100μm為佳,較佳為0.5~50μm,更佳為0.5~30μm。
而且,針對使用上述塗佈法或薄膜層積法所形成的樹脂膜,進行交聯反應。此種交聯係按照交聯劑(C)的種類而選擇適當的方法即可,通常藉由加熱而進行。
加熱方法係例如能夠使用加熱板、烘箱等而進行。加熱溫度係通常150~250℃,加熱時間係依照樹脂膜的面積和厚度、使用機器等而適當地選擇,例如使用加熱板時,通常為5~60分鐘,使用烘箱時,通常為30~300分鐘的範圍。必要時,可
在惰性氣體環境下進行加熱。作為惰性氣體,係不含有氧且不使樹脂膜氧化者即可,例如可舉出氮、氬、氦、氖、氙、氪等。該等之中,以氮及氬為佳,以氮為特佳。特別是氧含量為0.1體積%以下,較佳為0.01體積%以下的惰性氣體,以氮為特佳。該等惰性氣體係各自能夠單獨、或組合2種以上而使用。
又,必要時,可圖案化由樹脂組合物所構成之樹脂膜。作為將樹脂膜圖案化之方法,例如可舉出使樹脂組合物含有光酸產生劑(D),使用含有光酸產生劑(D)之樹脂組合物而形成圖案化前的樹脂膜,而且對圖案化前的樹脂膜照射活性放射線而形成潛像圖案,其次,藉由使顯影液接觸具有潛像圖案的樹脂膜,使圖案顯在之方法等。或者,使用光酸產生劑(D)來圖案化以外之方法,亦能夠使用下述等:使用雷射加工之方法,該方法係使用CO2雷射、UV-YAG雷射等;或在樹脂膜上形成光罩圖案而進行乾蝕刻之方法;以及噴墨法等的直接描繪法。
作為活性放射線,只要使在樹脂組合物所含有的光酸產生劑(D)活性化,且能夠使含有光酸產生劑(D)的樹脂組合物之鹼可溶性產生變化者,就沒有特別限定。具體而言,能夠使用紫外線、g-h-i射線等單一波長的紫外線、KrF準分子雷射光、ArF準分子雷射光等的光線;如電子射線的粒子線等。作為選擇性對該等活性放射線圖案狀地照射,而形成潛像圖案之方法,係依照常用的方法即可,例如能夠使用縮小投影曝光裝置等,透過所需要的光罩圖案而照射紫外線、g-h-i射線、KrF準分子雷射光、ArF準分子雷射光等的光線、或使用電子射線等的粒子線進行描繪之方法等。使用光線作為活性放射線
時,可為單一波長光、亦可為混合波長光。照射條件係按照所使用的活性放射線而適當地選擇,例如使用波長200~450nm的光線時,照射量係通常10~1,000mJ/cm2,較佳為50~500mJ/cm2的範圍,可按照照射時間及照度而決定。如此進行而照射活性放射線之後,必要時,在60~130℃左右的溫度將樹脂膜進行加熱處理1~2分鐘左右。
其次,使形成在圖案化前的樹脂膜上的潛像圖案顯影而顯在化。作為顯影液,通常能夠使用鹼性化合物的水性溶液。作為鹼性化合物,例如能夠使用鹼金屬鹽、胺、銨鹽。鹼性化合物可為無機化合物,亦可為有機化合物。作為該等化合物的具體例,可舉出氫氧化鈉、氫氧化鉀、碳酸鈉、矽酸鈉、偏矽酸鈉等的鹼金屬鹽;氨水;乙胺、正丙基胺等的第一級胺;二乙胺、二-正丙基胺等的第二級胺;三乙胺、甲基二乙胺等的第三級胺;氫氧化四甲銨、氫氧化四乙銨、氫氧化四丁銨、膽鹼等的第四級銨鹽;二甲基乙醇胺、三乙醇胺等的醇類胺;吡咯、哌啶、1,8-二氮雜雙環[5.4.0]十一-7-烯、1,5-二氮雜雙環[4.3.0]九-5-烯、N-甲基吡咯啶酮等的環狀胺類等。該等鹼性化合物係各自能夠單獨、或組合2種以上而使用。
作為鹼性水溶液的水性介質,能夠使用水;甲醇、乙醇等的水溶性有機溶劑。鹼性水溶液亦可為添加有適當量的界面活性劑等而成者。
作為使顯影液接觸具有潛像圖案的樹脂膜之方法,例如能夠使用浸置(puddle)法、噴霧法、浸漬法等的方法。顯影係通常為0~100℃,以5~55℃為佳,較佳為10~30℃的範圍,通常
能夠適當地在30~180秒鐘的範圍選擇。
如此進行而形成有目標圖案之樹脂膜,係為了必要時,將顯影殘渣除去,而能夠使用沖洗液進行沖洗。沖洗處理之後,係使用壓縮空氣和壓縮氮氣將殘留的沖洗液除去。
而且,為了必要時,使在樹脂組合物所含有的光酸產生劑(D)失去活性,亦能夠對電子元件全面照射活性放射線。活性放射線的照射係能夠利用在上述形成潛像圖案已例示的方法。亦可在照射之同時或照射後,將樹脂膜進行加熱。作為加熱方法,例如可舉出在加熱板和烘箱內加熱電子元件之方法。溫度係通常100~300℃,較佳為120~200℃的範圍。
在本發明,樹脂膜係在圖案化之後,能夠進行交聯反應。交聯係依照上述的方法進行即可。
因為本發明的樹脂組合物,係含有黏結劑樹脂(A)、羥基當量為300以上的苯氧基樹脂(B)及交聯劑(C),所以使用此種本發明的樹脂組合物而得到的樹脂膜,係具有優異的耐熱性、對基板的密著性、焊料耐熱性、及耐熱衝擊性者。因此,使用此種本發明的樹脂組合物而得到的樹脂膜,係能夠適合使用在電子元件、特別是藉由晶圓等級封裝技術而製造之電子元件。
[實施例]
以下,舉出實施例及比較例而更具體地說明本發明。各例中的「份」係只要未預先告知,就是重量基準。
又,各特性的定義及評價方法係如以下。
<耐熱性>
使用濺鍍裝置,對形成有100nm膜厚之鋁薄膜的矽晶圓上,將樹脂組合物進行旋轉塗佈之後,使用加熱板在120℃加熱2分鐘,其次,在氮氣環境下藉由於200℃且60分鐘的條件下使其硬化,而形成膜厚10μm的樹脂膜來得到積層體。而且,藉由將所得到的積層體切斷成為預定大小後,使鋁薄膜溶解在0.1mol/L的鹽酸水溶液而使其剝離,且使剝離後的薄膜乾燥,來得到樹脂膜。而且,針對所得到的樹脂膜,使用黏彈性分光儀(SII NanoTechnology公司、DMS6100標準型)而測定樹脂膜的玻璃轉移溫度(℃),基於以下的基準而進行評價耐熱性。玻璃轉移溫度越高,能夠判定具有優異的耐熱性。
A:玻璃轉移溫度為160℃以上
B:玻璃轉移溫度為150℃以上且小於160℃
C:玻璃轉移溫度小於150℃
<對基板的密著性>
使用濺鍍裝置在50nm厚的鈦膜上,形成有100nm膜厚的銅之矽晶圓上,將樹脂組合物旋轉塗佈之後,使用加熱板於120℃加熱2分鐘,其次,藉由在氮氣環境下於200℃且60分鐘的條件下使其硬化,經由形成膜厚10μm的樹脂膜而得到積層體。然後,針對形成積層體之樹脂膜進行橫切試驗。具體而言,首先使用切刀對形成積層體之樹脂膜,以1mm×1mm的大小形成10×10=100個棋盤格。而且,將玻璃紙膠黏帶強勁地壓黏在棋盤格部分且將玻璃紙膠黏帶(Cellophane tape)的端部以45°的角度一口氣地剝下,而求取樹脂膜的殘留比例(在使用濺鍍裝置在50nm厚的鈦膜上,形成有100nm膜厚的銅之矽晶圓上所殘留
的樹脂膜之比例),基於以下的基準對基板的密著性進行評價。
A:樹脂膜的殘留比例為90%以上
B:樹脂膜的殘留比例為80%以上且小於90%
C:樹脂膜的殘留比例小於80%
<焊料耐熱性>
在使用濺鍍裝置在50nm厚的鈦膜上,以100nm的膜厚形成有銅之矽晶圓上,將樹脂組合物旋轉塗佈之後,使用加熱板於120℃加熱2分鐘,其次藉由在氮氣環境下於200℃且60分鐘的條件下,使其硬化,且經由形成膜厚10μm的樹脂膜而得到積層體。在如此進行而得到的積層體之樹脂膜上,藉由濺鍍法而形成銅箔膜,其次,藉由使用含有硫酸銅之酸性水溶液作為電鍍浴之電鍍,以厚度10μm形成鍍銅層之後,於180℃進行加熱處理60分鐘而得到試片。而且,使所得到的試片在焊料溫度260℃的焊料浴浮起10秒鐘,且在室溫放置30秒鐘後,重複進行確保鍍銅層有無膨脹之試驗至能夠確認鍍銅層產生膨脹為止,依照以下的基準而進行評價焊料耐熱性。至能夠確認鍍銅層產生膨脹為止的試驗重複次數越多,能夠判定具有優異的焊料耐熱性。
A:重複進行上述試驗10次,但是第10次的試驗後亦無法確認鍍銅層產生膨脹。
B:至能夠確認鍍銅層產生膨脹為止的試驗重複次數為8次以上且10次以下。
C:至能夠確認鍍銅層產生膨脹為止的試驗重複次數為小於8次。
<耐熱衝擊性>
在矽晶圓上具有圖案狀銅配線之熱衝擊用評價基板上,將樹脂組合物進行旋轉塗佈之後,在氮氣環境下於120℃進行加熱2分鐘,其次,藉由在200℃且60分鐘的條件下使其硬化,而形成膜厚10μm的樹脂膜,來得到評價用樣品。而且,針對所得到的評價用樣品,使用熱衝擊試驗器(TABAI ESPEC公司製),將-55℃/30分鐘及150℃/30分鐘設作1循環,進行熱衝擊試驗至能夠確認在樹脂膜產生龜裂為止之循環數,基於以下的基準而進行評價耐熱衝擊性。
A:1000循環經過後亦不產生龜裂。
C:在1000循環到達前產生龜裂。
《合成例1》
<環狀烯烴聚合物(A-1)的調製>
將由N-苯基-雙環[2.2.1]庚-5-烯-2,3-二羧醯亞胺(NBPI)40莫耳%、及4-羥羰基四環[6.2.1.13,6.02,7]十二-9-烯(TCDC)60莫耳%所構成的單體混合物100份、1,5-己二烯2.0份、(1,3-二均三甲苯基咪唑-2-亞基)(三環己基膦)二氯化亞苄基釕(使用在有機通訊期刊Org.Lett.,第1卷,第953頁,1999年記載的方法合成而成)0.02份、及二乙二醇乙基甲醚200份,添加在經氮氣取代之玻璃製耐壓反應器,且邊攪拌邊在80℃使其反應4小時而得到聚合反應液。
然後,將所得到的聚合反應液添加至高壓釜,在150℃且氫壓4MPa攪拌5小時而進行氫化反應,來得到含有環狀烯烴聚合物(A-1)之聚合物溶液。所得到的環狀烯烴聚合
物(A-1)之聚合轉化率為99.7%,聚苯乙烯換算重量平均分子量為7,150,數量平均分子量為4,690,分子量分布為1.52,氫化率為99.7%。又,所得到的環狀烯烴聚合物(A-1)之聚合物溶液的固體成分濃度為34.4重量%。
《實施例1》
將作為黏結劑樹脂(A)之合成例1所得到的環狀烯烴聚合物(A-1)之聚合物溶液291份(環狀烯烴聚合物(A-1)為100份),作為苯氧基樹脂(B)之含雙酚S骨架的苯氧基樹脂(商品名「jER YX8100BH30」、三菱化學公司製、羥基當量308)25份、作為交聯劑(C)之環氧化丁烷四羧酸肆(3-環己烯基甲基)改性ε-己內酯(商品名「EPOLEAD GT401」、Daicel化學工業公司製、脂肪族環狀4官能性的環氧樹脂)30份、同樣地作為交聯劑(C)之長鏈雙酚A型環氧樹脂(商品名「EXA-4816」、DIC公司製)10份、同樣地作為交聯劑(C)之N,N,N’,N’,N”,N”-六甲氧基甲基三聚氰胺(商品名「Nikalac Mw-100LM」、三和Chemical公司製)15份、作為矽烷偶合劑之γ-環氧丙基丙基三甲氧基矽烷(商品名「Z6040」、TORAY‧DOW CORNING公司製)3份、及作為溶劑之二乙二醇乙基甲醚160份,進行混合且使其溶解後,使用孔徑0.45μm的聚四氟乙烯製過濾器過濾而調製樹脂組合物。
然後,使用所得到的樹脂組合物而進行耐熱性、對基板的密著性、焊料耐熱性、及耐熱衝擊性的各測定‧評價。將結果顯示在表1。
(實施例2~6》
除了將表1所顯示的化合物,使用表1所顯示的量以外,係與實施例1同樣地進行而調製樹脂組合物且同樣地進行評價。將結果顯示在表1。
《比較例1、2》
除了將表1所顯示的化合物,使用表1所顯示的量以外,係與實施例1同樣地進行而調製樹脂組合物,且同樣地進行評價。將結果顯示在表1。
又,表1中所顯示的各化合物係如以下。
‧黏結劑樹脂「環狀烯烴聚合物(A-1)」;製造例1所得到的環狀烯烴聚合物(A-1)
‧黏結劑樹脂「丙烯酸聚合物(MARUKALYNCUR CMM)」;丙烯酸聚合物(商品名「MARUKALYNCUR CMM」、丸善石油化學公司製、對羥基苯乙烯與甲基丙烯酸甲酯的共聚物)
‧苯氧基樹脂「jER YX8100BH30」;含雙酚S骨架的苯
氧基樹脂(商品名「jER YX8100BH30」、三菱化學公司製、羥基當量308)
‧苯氧基樹脂「jER YX6954BH30」;雙酚苯乙酮骨架含有苯氧基樹脂(商品名「jER YX6954BH30」、三菱化學公司製、羥基當量325)
‧苯氧基樹脂「jER 1256B40」;雙酚A骨架含有苯氧基樹脂(商品名「jER 1256B40」、三菱化學公司製、羥基當量284)
‧苯氧基樹脂「PhenoTohto YP-70」;雙酚A‧雙酚F共聚合苯氧基樹脂(商品名「PhenoTohto YP-70」、新日鐵柱金化學公司製、羥基當量270)
‧含有2個以上的烷氧基甲基、或羥甲基之化合物「Nikalac MW100LM」;N,N,N’,N’,N”,N”-六甲氧基甲基三聚氰胺(商品名「Nikalac MW-100LM」、三和Chemical公司製)
‧含有烷氧基甲基、或羥甲基的化合物;「TMOM-BP」;3,3’,5,5’-四甲氧基甲基-4,4’-雙酚(商品名「TMOM-BP」、本州化學工業公司製)
‧含有2個以上的烷氧基甲基、或羥甲基之化合物「HMOM-TPHAP-GB」;4,4’,4”-(亞乙基)參苯酚等的六甲氧基甲基取代化合物(商品名「HMOM-TPHAP-GB」、本州化學工業公司製)
‧含環氧基交聯劑「EPOLEAD GT401」;環氧化丁基四羧酸肆(3-環己烯基甲基)改性ε-己內酯(商品名「EPOLEAD GT401」、Daicel化學工業公司製、脂肪族環狀4官能性的環氧樹脂)
‧含環氧基交聯劑「EXA-4816」;長鏈雙酚A型環氧樹
脂(商品名「EXA-4816」、DIC公司製)
‧光酸產生劑「TS200」;4,4’-[1-[4-[1-[4-羥苯基]-1-甲基乙基]苯基]亞乙基]雙酚(1莫耳)與1,2-萘醌二疊氮-5-磺醯氯(2.0莫耳)的縮合物(商品名「TS200」、東洋合成股份公司製)
‧矽烷偶合劑「Z6040」;γ-環氧丙基丙基三甲氧基矽烷(商品名「Z6040」、TORAY‧DOW CORNING公司製)
‧矽烷偶合劑「Z6883」;3-苯胺基丙基三甲氧基矽烷(商品名「Z6883」、TORAY‧DOW CORNING公司製)
如表1所顯示,使用含有黏結劑樹脂(A)、羥基當量為300以上的苯氧基樹脂(B)、及交聯劑(C)之樹脂組合物而得到的樹脂膜,係耐熱性、對基板的密著性、焊料耐熱性、及耐熱衝擊性的任一者均優異者(實施例1~6)。
另一方面,使用羥基當量小於300的羥基當量之情況,所得到的樹脂膜係耐熱性及焊料耐熱性較差者(比較例1)。
又,未混合羥基當量為300以上的苯氧基樹脂(B)之情況,所得到的樹脂膜,係對基板的密著性、焊料耐熱性、及耐熱衝擊性較差者(比較例2)。
Claims (10)
- 一種樹脂組合物,係含有黏結劑樹脂(A)、羥基當量為300以上的苯氧基樹脂(B)及交聯劑(C),其中前述交聯劑(C)係在分子內含有2個以上的烷氧基甲基或羥甲基之化合物、或者脂環式環氧化合物。
- 如申請專利範圍第1項所述之樹脂組合物,其中相對於形成前述樹脂組合物之固體成分全體,以80重量%以下的含量含有填料。
- 如申請專利範圍第2項所述之樹脂組合物,其中相對於形成前述樹脂組合物之固體成分全體,前述填料的含量為0重量%。
- 如申請專利範圍第1至3項中任一項所述之樹脂組合物,其中前述交聯劑(C)係在分子內含有2個以上的烷氧基甲基或羥甲基之化合物及脂環式環氧化合物。
- 如申請專利範圍第1至3項中任一項所述之樹脂組合物,更含有光酸產生劑(D)。
- 如申請專利範圍第5項所述之樹脂組合物,其中前述光酸產生劑(D)為醌二疊氮化合物。
- 如申請專利範圍第1至3項中任一項所述之樹脂組合物,其中前述黏結劑樹脂(A)為具有質子性極性基的環狀烯烴聚合物。
- 如申請專利範圍第1至3項中任一項所述之樹脂組合物,其中相對於形成前述樹脂組合物之固體成分全體,前述苯氧基樹脂(B)的含有比例為2~75重量%。
- 如申請專利範圍第1至3項中任一項所述之樹脂組合物,其中前述苯氧基樹脂(B)係具備雙酚結構之苯氧基樹脂。
- 一種電子元件,係具備由如申請專利範圍第1至3項中任一項所述之樹脂組合物所構成之樹脂膜。
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