JP6825368B2 - 銅張積層体及びプリント配線板 - Google Patents
銅張積層体及びプリント配線板 Download PDFInfo
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- JP6825368B2 JP6825368B2 JP2017000250A JP2017000250A JP6825368B2 JP 6825368 B2 JP6825368 B2 JP 6825368B2 JP 2017000250 A JP2017000250 A JP 2017000250A JP 2017000250 A JP2017000250 A JP 2017000250A JP 6825368 B2 JP6825368 B2 JP 6825368B2
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- copper
- clad laminate
- bis
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- -1 aromatic tetracarboxylic acid Chemical class 0.000 claims description 42
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 35
- 229920005989 resin Polymers 0.000 claims description 29
- 239000011347 resin Substances 0.000 claims description 29
- 150000004985 diamines Chemical class 0.000 claims description 28
- 239000011889 copper foil Substances 0.000 claims description 27
- 239000012790 adhesive layer Substances 0.000 claims description 20
- 239000000539 dimer Substances 0.000 claims description 18
- 229920001721 polyimide Polymers 0.000 claims description 15
- 239000004643 cyanate ester Substances 0.000 claims description 11
- 239000000178 monomer Substances 0.000 claims description 11
- 239000004642 Polyimide Substances 0.000 claims description 10
- XQUPVDVFXZDTLT-UHFFFAOYSA-N 1-[4-[[4-(2,5-dioxopyrrol-1-yl)phenyl]methyl]phenyl]pyrrole-2,5-dione Chemical compound O=C1C=CC(=O)N1C(C=C1)=CC=C1CC1=CC=C(N2C(C=CC2=O)=O)C=C1 XQUPVDVFXZDTLT-UHFFFAOYSA-N 0.000 claims description 8
- 229920003192 poly(bis maleimide) Polymers 0.000 claims description 7
- 229920001955 polyphenylene ether Polymers 0.000 claims description 7
- CMLFRMDBDNHMRA-UHFFFAOYSA-N 2h-1,2-benzoxazine Chemical compound C1=CC=C2C=CNOC2=C1 CMLFRMDBDNHMRA-UHFFFAOYSA-N 0.000 claims description 5
- 238000004132 cross linking Methods 0.000 claims description 5
- 150000008065 acid anhydrides Chemical group 0.000 claims description 3
- 239000007795 chemical reaction product Substances 0.000 claims description 3
- XBTRYWRVOBZSGM-UHFFFAOYSA-N (4-methylphenyl)methanediamine Chemical compound CC1=CC=C(C(N)N)C=C1 XBTRYWRVOBZSGM-UHFFFAOYSA-N 0.000 claims description 2
- 125000000596 cyclohexenyl group Chemical group C1(=CCCCC1)* 0.000 claims description 2
- 125000000843 phenylene group Chemical group C1(=C(C=CC=C1)*)* 0.000 claims description 2
- 238000012545 processing Methods 0.000 claims description 2
- AHIPJALLQVEEQF-UHFFFAOYSA-N 4-(oxiran-2-ylmethoxy)-n,n-bis(oxiran-2-ylmethyl)aniline Chemical compound C1OC1COC(C=C1)=CC=C1N(CC1OC1)CC1CO1 AHIPJALLQVEEQF-UHFFFAOYSA-N 0.000 claims 1
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 36
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- 229920000647 polyepoxide Polymers 0.000 description 28
- 239000000203 mixture Substances 0.000 description 24
- 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 description 19
- 239000000243 solution Substances 0.000 description 18
- 239000000853 adhesive Substances 0.000 description 16
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- 230000000052 comparative effect Effects 0.000 description 13
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- JHIVVAPYMSGYDF-UHFFFAOYSA-N cyclohexanone Chemical compound O=C1CCCCC1 JHIVVAPYMSGYDF-UHFFFAOYSA-N 0.000 description 12
- UAEPNZWRGJTJPN-UHFFFAOYSA-N methylcyclohexane Chemical compound CC1CCCCC1 UAEPNZWRGJTJPN-UHFFFAOYSA-N 0.000 description 12
- 239000000047 product Substances 0.000 description 12
- 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 11
- 238000006243 chemical reaction Methods 0.000 description 11
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- 239000004205 dimethyl polysiloxane Substances 0.000 description 7
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- 229920000435 poly(dimethylsiloxane) Polymers 0.000 description 7
- 125000006158 tetracarboxylic acid group Chemical group 0.000 description 7
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 6
- 239000011248 coating agent Substances 0.000 description 6
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- 125000003118 aryl group Chemical group 0.000 description 5
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- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 4
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 4
- ATUOYWHBWRKTHZ-UHFFFAOYSA-N Propane Chemical compound CCC ATUOYWHBWRKTHZ-UHFFFAOYSA-N 0.000 description 4
- USIUVYZYUHIAEV-UHFFFAOYSA-N diphenyl ether Natural products C=1C=CC=CC=1OC1=CC=CC=C1 USIUVYZYUHIAEV-UHFFFAOYSA-N 0.000 description 4
- KZTYYGOKRVBIMI-UHFFFAOYSA-N diphenyl sulfone Chemical compound C=1C=CC=CC=1S(=O)(=O)C1=CC=CC=C1 KZTYYGOKRVBIMI-UHFFFAOYSA-N 0.000 description 4
- 125000000524 functional group Chemical group 0.000 description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- ZWEHNKRNPOVVGH-UHFFFAOYSA-N 2-Butanone Chemical compound CCC(C)=O ZWEHNKRNPOVVGH-UHFFFAOYSA-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
- WFDIJRYMOXRFFG-UHFFFAOYSA-N Acetic anhydride Chemical compound CC(=O)OC(C)=O WFDIJRYMOXRFFG-UHFFFAOYSA-N 0.000 description 3
- WVDDGKGOMKODPV-UHFFFAOYSA-N Benzyl alcohol Chemical compound OCC1=CC=CC=C1 WVDDGKGOMKODPV-UHFFFAOYSA-N 0.000 description 3
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 description 3
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 3
- 229920000106 Liquid crystal polymer Polymers 0.000 description 3
- 239000004977 Liquid-crystal polymers (LCPs) Substances 0.000 description 3
- IMYZQPCYWPFTAG-UHFFFAOYSA-N Mecamylamine Chemical compound C1CC2C(C)(C)C(NC)(C)C1C2 IMYZQPCYWPFTAG-UHFFFAOYSA-N 0.000 description 3
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 3
- LGRFSURHDFAFJT-UHFFFAOYSA-N Phthalic anhydride Natural products C1=CC=C2C(=O)OC(=O)C2=C1 LGRFSURHDFAFJT-UHFFFAOYSA-N 0.000 description 3
- 229910000831 Steel Inorganic materials 0.000 description 3
- ZMANZCXQSJIPKH-UHFFFAOYSA-N Triethylamine Chemical compound CCN(CC)CC ZMANZCXQSJIPKH-UHFFFAOYSA-N 0.000 description 3
- 239000000654 additive Substances 0.000 description 3
- 125000003236 benzoyl group Chemical group [H]C1=C([H])C([H])=C(C([H])=C1[H])C(*)=O 0.000 description 3
- PXKLMJQFEQBVLD-UHFFFAOYSA-N bisphenol F Chemical compound C1=CC(O)=CC=C1CC1=CC=C(O)C=C1 PXKLMJQFEQBVLD-UHFFFAOYSA-N 0.000 description 3
- JHIWVOJDXOSYLW-UHFFFAOYSA-N butyl 2,2-difluorocyclopropane-1-carboxylate Chemical compound CCCCOC(=O)C1CC1(F)F JHIWVOJDXOSYLW-UHFFFAOYSA-N 0.000 description 3
- 125000004432 carbon atom Chemical group C* 0.000 description 3
- 239000007809 chemical reaction catalyst Substances 0.000 description 3
- 239000004020 conductor Substances 0.000 description 3
- 229910052802 copper Inorganic materials 0.000 description 3
- 239000010949 copper Substances 0.000 description 3
- 229930003836 cresol Natural products 0.000 description 3
- 239000000945 filler Substances 0.000 description 3
- 239000011521 glass Substances 0.000 description 3
- 150000002430 hydrocarbons Chemical class 0.000 description 3
- 238000005065 mining Methods 0.000 description 3
- PHQOGHDTIVQXHL-UHFFFAOYSA-N n'-(3-trimethoxysilylpropyl)ethane-1,2-diamine Chemical compound CO[Si](OC)(OC)CCCNCCN PHQOGHDTIVQXHL-UHFFFAOYSA-N 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N nitrogen Substances N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 3
- 125000000951 phenoxy group Chemical group [H]C1=C([H])C([H])=C(O*)C([H])=C1[H] 0.000 description 3
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 description 3
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- 229920006259 thermoplastic polyimide Polymers 0.000 description 3
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- CQOZJDNCADWEKH-UHFFFAOYSA-N 2-[3,3-bis(2-hydroxyphenyl)propyl]phenol Chemical compound OC1=CC=CC=C1CCC(C=1C(=CC=CC=1)O)C1=CC=CC=C1O CQOZJDNCADWEKH-UHFFFAOYSA-N 0.000 description 2
- KRPRVQWGKLEFKN-UHFFFAOYSA-N 3-(3-aminopropoxy)propan-1-amine Chemical compound NCCCOCCCN KRPRVQWGKLEFKN-UHFFFAOYSA-N 0.000 description 2
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- RSWGJHLUYNHPMX-UHFFFAOYSA-N Abietic-Saeure Natural products C12CCC(C(C)C)=CC2=CCC2C1(C)CCCC2(C)C(O)=O RSWGJHLUYNHPMX-UHFFFAOYSA-N 0.000 description 2
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- IAZDPXIOMUYVGZ-UHFFFAOYSA-N Dimethylsulphoxide Chemical compound CS(C)=O IAZDPXIOMUYVGZ-UHFFFAOYSA-N 0.000 description 2
- FXHOOIRPVKKKFG-UHFFFAOYSA-N N,N-Dimethylacetamide Chemical compound CN(C)C(C)=O FXHOOIRPVKKKFG-UHFFFAOYSA-N 0.000 description 2
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- QLBRROYTTDFLDX-UHFFFAOYSA-N [3-(aminomethyl)cyclohexyl]methanamine Chemical compound NCC1CCCC(CN)C1 QLBRROYTTDFLDX-UHFFFAOYSA-N 0.000 description 2
- 125000004018 acid anhydride group Chemical group 0.000 description 2
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- IPJGAEWUPXWFPL-UHFFFAOYSA-N 1-[3-(2,5-dioxopyrrol-1-yl)phenyl]pyrrole-2,5-dione Chemical compound O=C1C=CC(=O)N1C1=CC=CC(N2C(C=CC2=O)=O)=C1 IPJGAEWUPXWFPL-UHFFFAOYSA-N 0.000 description 1
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- 239000010935 stainless steel Substances 0.000 description 1
- 239000008117 stearic acid Substances 0.000 description 1
- 235000021286 stilbenes Nutrition 0.000 description 1
- 229940014800 succinic anhydride Drugs 0.000 description 1
- 239000012756 surface treatment agent Substances 0.000 description 1
- 230000008961 swelling Effects 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 238000010345 tape casting Methods 0.000 description 1
- GJBRNHKUVLOCEB-UHFFFAOYSA-N tert-butyl benzenecarboperoxoate Chemical compound CC(C)(C)OOC(=O)C1=CC=CC=C1 GJBRNHKUVLOCEB-UHFFFAOYSA-N 0.000 description 1
- 150000003512 tertiary amines Chemical class 0.000 description 1
- 238000010998 test method Methods 0.000 description 1
- LPSXSORODABQKT-UHFFFAOYSA-N tetrahydrodicyclopentadiene Chemical compound C1C2CCC1C1C2CCC1 LPSXSORODABQKT-UHFFFAOYSA-N 0.000 description 1
- 230000000930 thermomechanical effect Effects 0.000 description 1
- 125000003396 thiol group Chemical group [H]S* 0.000 description 1
- 150000003573 thiols Chemical group 0.000 description 1
- 229910052718 tin Inorganic materials 0.000 description 1
- PJANXHGTPQOBST-VAWYXSNFSA-N trans-stilbene Chemical compound C=1C=CC=CC=1/C=C/C1=CC=CC=C1 PJANXHGTPQOBST-VAWYXSNFSA-N 0.000 description 1
- TUQOTMZNTHZOKS-UHFFFAOYSA-N tributylphosphine Chemical compound CCCCP(CCCC)CCCC TUQOTMZNTHZOKS-UHFFFAOYSA-N 0.000 description 1
- JXUKBNICSRJFAP-UHFFFAOYSA-N triethoxy-[3-(oxiran-2-ylmethoxy)propyl]silane Chemical compound CCO[Si](OCC)(OCC)CCCOCC1CO1 JXUKBNICSRJFAP-UHFFFAOYSA-N 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
- DQZNLOXENNXVAD-UHFFFAOYSA-N trimethoxy-[2-(7-oxabicyclo[4.1.0]heptan-4-yl)ethyl]silane Chemical compound C1C(CC[Si](OC)(OC)OC)CCC2OC21 DQZNLOXENNXVAD-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
- KLNPWTHGTVSSEU-UHFFFAOYSA-N undecane-1,11-diamine Chemical compound NCCCCCCCCCCCN KLNPWTHGTVSSEU-UHFFFAOYSA-N 0.000 description 1
- 235000021122 unsaturated fatty acids Nutrition 0.000 description 1
- 150000004670 unsaturated fatty acids Chemical class 0.000 description 1
- 239000004034 viscosity adjusting agent Substances 0.000 description 1
- 239000008096 xylene Substances 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B15/00—Layered products comprising a layer of metal
- B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B15/00—Layered products comprising a layer of metal
- B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
- B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B15/00—Layered products comprising a layer of metal
- B32B15/20—Layered products comprising a layer of metal comprising aluminium or copper
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B7/00—Layered products characterised by the relation between layers; Layered products characterised by the relative orientation of features between layers, or by the relative values of a measurable parameter between layers, i.e. products comprising layers having different physical, chemical or physicochemical properties; Layered products characterised by the interconnection of layers
- B32B7/02—Physical, chemical or physicochemical properties
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B7/00—Layered products characterised by the relation between layers; Layered products characterised by the relative orientation of features between layers, or by the relative values of a measurable parameter between layers, i.e. products comprising layers having different physical, chemical or physicochemical properties; Layered products characterised by the interconnection of layers
- B32B7/04—Interconnection of layers
- B32B7/12—Interconnection of layers using interposed adhesives or interposed materials with bonding properties
-
- 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
- H05K1/00—Printed circuits
- H05K1/02—Details
- H05K1/03—Use of materials for the substrate
- H05K1/0313—Organic insulating material
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2307/00—Properties of the layers or laminate
- B32B2307/20—Properties of the layers or laminate having particular electrical or magnetic properties, e.g. piezoelectric
- B32B2307/206—Insulating
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2307/00—Properties of the layers or laminate
- B32B2307/30—Properties of the layers or laminate having particular thermal properties
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2307/00—Properties of the layers or laminate
- B32B2307/50—Properties of the layers or laminate having particular mechanical properties
- B32B2307/538—Roughness
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2311/00—Metals, their alloys or their compounds
- B32B2311/24—Aluminium
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2457/00—Electrical equipment
- B32B2457/08—PCBs, i.e. printed circuit boards
Description
項1. 絶縁フィルム(1)の少なくとも片側の面に接着剤層(2)を介して積層された銅箔(3)を備えた銅張積層体であり、
(1)の熱膨張係数が4〜30ppm/℃であり、
(2)が、芳香族テトラカルボン酸無水物及びダイマージアミンを含むジアミンモノマーの反応物である酸無水物基末端ポリイミド(A)と架橋成分(B)を含有し、
(3)の(2)と接する面の十点平均粗さ(Rz)が、0.1〜1.5μmである銅張積層体である。
2−メチルイミダゾール、2−フェニルイミダゾール、2−フェニル−4−メチルイミダゾール、2−エチル−4−メチルイミダゾール、1−シアノエチルー2−ウンデシルイミダゾール、2−ヘプタデシルイミダゾール等のイミダゾ−ル類;
トリブチルホスフィン、メチルジフェニルホスフィン、トリフェニルホスフィン、ジフェニルホスフィン、フェニルホスフィン等の有機ホスフィン類;
テトラフェニルホスホニウム・テトラフェニルボレート、2−エチル−4−メチルイミダゾール・テトラフェニルボレート、N−メチルモルホリン・テトラフェニルボレート等のテトラフェニルボロン塩;オクタン酸、ステアリン酸、アセチルアセトネート、ナフテン酸、及びサリチル酸等の有機酸のZn、Cu、及びFe等の有機金属塩;
ベンゾイルパーオキサイド、メチルエチルケトンパーオキサイド、シクロヘキサノンパーオキサイド、ラウロイルパーオキサイド、ジ−t−ブチルパーオキサイド、t−ブチルパーベンゾエート、クメンハイドロパーオキサイド、ジクミルパーオキサイド等のラジカル開始剤等が挙げられ、二種以上組み合わせてもよい。また、当該触媒の使用量は特に制限されないが、通常、本発明の接着剤組成物の固形分を100重量%として0.01〜5重量%程度である。
乾燥方法は、好ましくは40〜250℃、より好ましくは70〜170℃で2〜15分間程度、熱風乾燥、遠赤外線加熱、高周波誘導加熱等の炉を通す方法が使用できる。
貼り合わせ方法は、好ましくは40〜250℃、より好ましくは50〜200℃の温度でロールラミネーター、熱プレスを行う方法が使用できる。
アフターキュアは、120〜250℃の温度、好ましくは70℃〜200℃で30分〜48時間程度、熱風乾燥、遠赤外線加熱、高周波誘導加熱等の炉を通す方法が使用できる。
接着剤層(2)の膜厚は、接着性、耐熱性、塗工の容易性、溶剤残留の危険性を考慮すると、1〜70μm程度が好ましい。
(A)成分の溶液1gを秤量し、180℃の循風乾燥機で60分乾燥し、乾燥前後の重量から式1により、不揮発分を算出した。
(式1)=(乾燥後の重量(g))/(乾燥前の重量(g))×100(%)
撹拌機、分水器、温度計及び窒素ガス導入管を備えた反応容器に、市販の芳香族テトラカルボン酸二無水物(商品名「BTDA−UP」、エボニックジャパン(株)製;3,3’,4,4’−ベンゾフェノンテトラカルボン酸二無水物の含有量が99.8%以上)210.0g、シクロヘキサノン1008.0g、メチルシクロヘキサン201.6gを仕込み、溶液を60℃まで加熱した。次いで、水添ダイマージアミン(商品名「PRIAMINE 1075」、クローダジャパン(株)製)341.7gを滴下した後、140℃で10時間かけてイミド化反応させることにより、軟化点約80℃及び重量平均分子量35,000のポリイミド樹脂(A−1)の溶液(不揮発分33.9%)を得た。なお、全ジアミンモノマー中のダイマージアミンの含有量は100モル%、酸成分/アミン成分のモル比は1.03であった。
製造例1と同様の反応容器に、市販の芳香族テトラカルボン酸二無水物(商品名「BisDA1000」、エボニックジャパン(株)製;4,4’−[プロパン−2,2−ジイルビス(1,4−フェニレンオキシ)]ジフタル酸二無水物の含有量が98.0%) 297.8g、シクロヘキサノン818.95g、メチルシクロヘキサン136.49gを仕込み、溶液を60℃まで加熱した。次いで、PRIAMINE 1075 200.28g、及び1,3−ビスアミノメチルシクロヘキサン24.83gを滴下した後、140℃で10時間かけてイミド化反応させることにより、軟化点約100℃及び重量平均分子量28,000のポリイミド(A−2)の溶液(不揮発分32.2%)を得た。なお、全ジアミンモノマー中のダイマージアミンの含有量は68モル%、酸成分/アミン成分のモル比は1.05であった。
撹拌機、分水器、温度計及び窒素ガス導入管を備えた反応容器に、市販の芳香族テトラカルボン酸二無水物(商品名「BisDA1000」、エボニックジャパン(株)製;4,4’−[プロパン−2,2−ジイルビス(1,4−フェニレンオキシ)]ジフタル酸二無水物の含有量が98.0%)200.00g、シクロヘキサノン700.00g、メチルシクロヘキサン175.00gを仕込み、溶液を60℃まで加熱した。次いで、水添ダイマージアミン(商品名「PRIAMINE 1075」、クローダジャパン(株)製)190.54gを滴下した後、140℃で10時間かけてイミド化反応させることにより、軟化点約80℃及び重量平均分子量22,000のポリイミド樹脂(A−3)の溶液(不揮発分30.2%)を得た。なお、全ジアミンモノマー中のダイマージアミンの含有量は100モル%、酸成分/アミン成分のモル比は1.03であった。
製造例1と同様の反応容器に、市販の芳香族テトラカルボン酸二無水物(商品名「BTDA−PF」、エボニックジャパン(株)製;3,3’,4,4’−ベンゾフェノンテトラカルボン酸二無水物の含有量が98%) 190.0g、シクロヘキサノン277.5g、メチルシクロヘキサン182.4gを仕込み、溶液を60℃まで加熱した。次いで、PRIAMINE 1075 277.5g、及びα,ω−ビス(3−アミノプロピル)ポリジメチルシロキサン(商品名「KF−8010」、信越化学工業(株)製)23.8gを滴下した後、140℃で10時間かけてイミド化反応させることにより、軟化点約70℃及び重量平均分子量18,000のポリイミド(A−4)の溶液(不揮発分30.8%)を得た。なお、全ジアミンモノマー中のダイマージアミンの含有量は95モル%、酸成分/アミン成分のモル比は1.09であった。
(A−1)成分の溶液10.20g、(A−2)成分の溶液10.74g、(A−3)成分の溶液5.72g、(B)成分としてN,N−ジグリシジル−4−グリシジルオキシアニリン(商品名「jER630」、三菱化学(株)製)0.27g及びシアネートエステル樹脂(商品名「TA」、三菱化学ガス(株)製)のメチルエチルケトン溶液(不揮発分40%)0.48g、N−2−(アミノエチル)−3−アミノプロピルトリメトキシシラン(商品名「KBM−603」、信越化学工業(株)製)のトルエン溶液(不揮発分10%)0.18g、希釈溶剤としてトルエン2.81gを混合し、不揮発分30.0%の接着剤組成物を得た。なお、(A)成分合成で使用された全ジアミンモノマー中のダイマージアミンの含有量は87.2モル%である。
表1又は表2に示す組成で接着剤組成物を得た。
接着剤組成物として、カルボキシNBR(商品名「XER−32C」、JSR(株)製)を用いた。
接着剤組成物として、アクリルエラストマー(商品名「SG−708−6」、ナガセケムテックス(株)製)を用いた。
実施例1〜13、比較例1〜3
配合例1〜13及び比較配合例1〜3の接着剤組成物を、圧延銅箔(商品名「GHF5」、JX金属(株)製、十点平均粗さ(Rz):0.45μm)に、乾燥後の厚みが12μmとなるようギャップコーターにて塗布した後、150℃で10分間乾燥させることによって樹脂付き銅箔を得た。この樹脂付き銅箔2枚を用いて、接着剤面が内側となるようにして、120℃で10分間除湿したポリイミドフィルム(商品名「カプトン100EN」、東レ・デユポン(株)製;膜厚25μm;熱膨張係数;15ppm/℃)を挟み込み、170℃、3MPaで30分間熱ラミネートすることで、銅張積層体を得た。
接着剤層がない銅張積層体として、パナソニック製R−F705(クラレ(株)製のLCP「ベクスター」の両面に圧延銅箔を300℃でラミネートしたもの)を用いた。
接着剤層がない銅張積層体として、パナソニック製R−F775(宇部興産(株)製のポリイミド「Upilex−VT」(熱可塑性ポリイミド層/非熱可塑性ポリイミド層/熱可塑性ポリイミド層の3層で構成)の両面に圧延銅箔を300℃でラミネートしたもの)を用いた。
配合例1〜13の接着剤組成物を、フッ素樹脂PFA平皿(直径75mm、(株)相互理化学硝子製作所製)に7g注ぎ、30℃×10時間、70℃×10時間、100℃×6時間、120℃×6時間、150℃×6時間、180℃×12時間の条件で硬化させることによって、膜厚約300μmの硬化物シートを得た。次いで、該硬化物シートについて、JIS C2565に準じ、10GHzにおける誘電率及び誘電正接を、市販の誘電率測定装置(空洞共振器タイプ、エーイーティー製)を用いて測定した。比較配合例1〜5の物性値は、カタログ値を参照した。表1及び表2に結果を示す(以下同様)。
実施例1〜13の銅張積層体について、JIS C−6481(フレキシブルプリント配線板用銅張積層板試験方法)に準じ、引き剥がし強さ(N/mm)を測定した。比較例の物性値は、カタログ値を参照した。
実施例1〜13及び比較例1〜5の銅張積層体について、硬化後、288℃のはんだ浴に銅箔側を下にして30秒浮かべ、外観変化の有無を確認した。変化がない場合は○、発泡、膨れがある場合を×とした。
実施例1〜13及び比較例1〜5の銅張積層体について、レジストパターンを形成した。次いで、濃度40%の塩化第二鉄水溶液への浸漬によって銅箔をエッチングすることにより、ライン長10cmの銅回路を作成した。
実施例1〜13及び比較例1〜5の回路評価用プリント配線板について、ネットワークアナライザ(商品名『E8363B』、Keysight Technologies製)を使用し、インピーダンスを50Ωに合わせ、10GHzの挿入(伝送)損失S21を測定した。
※1:(A)成分の重量平均分子量:(A−1)−35000、(A−2)−28000、(A−3)−22000、(A−4)−18000
※2:GHF5−JX金属(株)製、十点平均粗さ(Rz):0.45μm
BHFX改−JX金属(株)製、十点平均粗さ(Rz):0.90μm
※3:実施例1〜13では接着剤層の誘電率及び誘電正接を示す。
Claims (7)
- 絶縁フィルム(1)の少なくとも片側の面に接着剤層(2)を介して積層された銅箔(3)を備えた銅張積層体であり、
(1)の熱膨張係数が4〜30ppm/℃であり、
(2)が、芳香族テトラカルボン酸無水物及びダイマージアミンを含むジアミンモノマーの反応物である酸無水物基末端ポリイミド(A)と架橋成分(B)を含有し、
(3)の(2)と接する面の十点平均粗さ(Rz)が、0.1〜1.5μmであり、
(B)成分が、N,N−ジグリシジル−4−グリシジルオキシアニリン及び/又は下記構造のテトラグリシジルキシレンジアミンを含むことを特徴とする銅張積層体。
- ダイマージアミンの含有量が、ジアミンモノマー中の30モル%以上である請求項1の銅張積層体。
- 芳香族テトラカルボン酸無水物が、下記一般式で示されるものである請求項1又は2の銅張積層体。
- 架橋成分(B)が、ポリフェニレンエーテル樹脂、ベンゾオキサジン樹脂、ビスマレイミド樹脂及びシアネートエステル樹脂からなる群より選ばれる少なくとも一種を含む請求項1〜3のいずれかの銅張積層体。
- 接着剤層(2)が更に反応性アルコキシシリル化合物(C)を含有する請求項1〜4のいずれかの銅張積層体。
- 接着剤層(2)の10GHzにおける誘電率が3.0以下であり、誘電正接が0.005以下である請求項1〜5のいずれかの銅張積層体。
- 請求項1〜6のいずれかの銅張積層体の銅箔を配線回路加工して得られるプリント配線板。
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JP6261037B2 (ja) * | 2014-02-06 | 2018-01-17 | 古河電気工業株式会社 | 高周波回路用銅箔、銅張積層板及びプリント配線板 |
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WO2022201619A1 (ja) * | 2021-03-25 | 2022-09-29 | 日本化薬株式会社 | 熱硬化性樹脂組成物、硬化物、樹脂シート、プリプレグ、金属箔張積層板、多層プリント配線板、封止用材料、繊維強化複合材料、接着剤及び半導体装置 |
WO2022201620A1 (ja) * | 2021-03-25 | 2022-09-29 | 日本化薬株式会社 | 樹脂組成物、硬化物、樹脂シート、プリプレグ、金属箔張積層板、多層プリント配線板、封止用材料、繊維強化複合材料、接着剤及び半導体装置 |
JP7191276B1 (ja) * | 2021-03-25 | 2022-12-16 | 日本化薬株式会社 | 樹脂組成物、硬化物、樹脂シート、プリプレグ、金属箔張積層板、多層プリント配線板、封止用材料、繊維強化複合材料、接着剤及び半導体装置 |
JP7191275B1 (ja) * | 2021-03-25 | 2022-12-16 | 日本化薬株式会社 | 熱硬化性樹脂組成物、硬化物、樹脂シート、プリプレグ、金属箔張積層板、多層プリント配線板、封止用材料、繊維強化複合材料、接着剤及び半導体装置 |
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JP2017121807A (ja) | 2017-07-13 |
KR20170082130A (ko) | 2017-07-13 |
TW201736118A (zh) | 2017-10-16 |
CN107009697A (zh) | 2017-08-04 |
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