WO2022065496A1 - Adhesive film for circuit connection, composition containing inorganic filler, circuit connection structure and method of manufacturing same - Google Patents
Adhesive film for circuit connection, composition containing inorganic filler, circuit connection structure and method of manufacturing same Download PDFInfo
- Publication number
- WO2022065496A1 WO2022065496A1 PCT/JP2021/035445 JP2021035445W WO2022065496A1 WO 2022065496 A1 WO2022065496 A1 WO 2022065496A1 JP 2021035445 W JP2021035445 W JP 2021035445W WO 2022065496 A1 WO2022065496 A1 WO 2022065496A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- adhesive layer
- component
- circuit connection
- inorganic filler
- circuit
- Prior art date
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- 239000002313 adhesive film Substances 0.000 title claims abstract description 142
- 239000000203 mixture Substances 0.000 title claims abstract description 126
- 239000011256 inorganic filler Substances 0.000 title claims abstract description 81
- 229910003475 inorganic filler Inorganic materials 0.000 title claims abstract description 81
- 238000004519 manufacturing process Methods 0.000 title claims description 25
- 239000002245 particle Substances 0.000 claims abstract description 168
- 229920001187 thermosetting polymer Polymers 0.000 claims abstract description 41
- 238000009826 distribution Methods 0.000 claims abstract description 21
- 238000009825 accumulation Methods 0.000 claims abstract description 13
- 239000012790 adhesive layer Substances 0.000 claims description 251
- 229920005989 resin Polymers 0.000 claims description 50
- 239000011347 resin Substances 0.000 claims description 50
- 239000000758 substrate Substances 0.000 claims description 48
- 239000010410 layer Substances 0.000 claims description 42
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical group O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 39
- 229920003023 plastic Polymers 0.000 claims description 27
- 239000004033 plastic Substances 0.000 claims description 27
- 238000000034 method Methods 0.000 claims description 26
- 239000000945 filler Substances 0.000 claims description 19
- 239000000377 silicon dioxide Substances 0.000 claims description 18
- 230000001186 cumulative effect Effects 0.000 claims description 17
- 229920005992 thermoplastic resin Polymers 0.000 claims description 4
- 238000002788 crimping Methods 0.000 claims description 3
- NIXOWILDQLNWCW-UHFFFAOYSA-M Acrylate Chemical compound [O-]C(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-M 0.000 description 100
- -1 polyethylene terephthalate Polymers 0.000 description 41
- 150000001875 compounds Chemical class 0.000 description 34
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- 239000000853 adhesive Substances 0.000 description 21
- 230000001070 adhesive effect Effects 0.000 description 21
- 150000001252 acrylic acid derivatives Chemical class 0.000 description 19
- 239000011521 glass Substances 0.000 description 19
- 239000000126 substance Substances 0.000 description 18
- 239000010419 fine particle Substances 0.000 description 17
- 239000003960 organic solvent Substances 0.000 description 17
- IISBACLAFKSPIT-UHFFFAOYSA-N bisphenol A Chemical class C=1C=C(O)C=CC=1C(C)(C)C1=CC=C(O)C=C1 IISBACLAFKSPIT-UHFFFAOYSA-N 0.000 description 16
- 239000011248 coating agent Substances 0.000 description 16
- 238000000576 coating method Methods 0.000 description 16
- 229920000139 polyethylene terephthalate Polymers 0.000 description 16
- 239000005020 polyethylene terephthalate Substances 0.000 description 16
- 150000003254 radicals Chemical class 0.000 description 16
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 15
- 238000010438 heat treatment Methods 0.000 description 15
- ZWEHNKRNPOVVGH-UHFFFAOYSA-N 2-Butanone Chemical compound CCC(C)=O ZWEHNKRNPOVVGH-UHFFFAOYSA-N 0.000 description 14
- 239000010936 titanium Substances 0.000 description 13
- 239000002966 varnish Substances 0.000 description 12
- 239000004593 Epoxy Substances 0.000 description 11
- 239000000654 additive Substances 0.000 description 11
- 230000007547 defect Effects 0.000 description 11
- 238000002360 preparation method Methods 0.000 description 11
- 230000001588 bifunctional effect Effects 0.000 description 10
- 230000000052 comparative effect Effects 0.000 description 10
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- 230000000694 effects Effects 0.000 description 9
- 125000002723 alicyclic group Chemical group 0.000 description 8
- 125000003700 epoxy group Chemical group 0.000 description 8
- 238000010030 laminating Methods 0.000 description 8
- 229910052751 metal Inorganic materials 0.000 description 8
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- 238000002156 mixing Methods 0.000 description 8
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- 229910052799 carbon Inorganic materials 0.000 description 7
- 238000005259 measurement Methods 0.000 description 7
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- 238000006243 chemical reaction Methods 0.000 description 5
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- 239000003822 epoxy resin Substances 0.000 description 5
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- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical class [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 4
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- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 4
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- 125000003566 oxetanyl group Chemical group 0.000 description 4
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- RPNUMPOLZDHAAY-UHFFFAOYSA-N Diethylenetriamine Chemical compound NCCNCCN RPNUMPOLZDHAAY-UHFFFAOYSA-N 0.000 description 3
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- 125000003118 aryl group Chemical group 0.000 description 3
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- MTHSVFCYNBDYFN-UHFFFAOYSA-N diethylene glycol Chemical compound OCCOCCO MTHSVFCYNBDYFN-UHFFFAOYSA-N 0.000 description 3
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- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 description 3
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- PUPZLCDOIYMWBV-UHFFFAOYSA-N (+/-)-1,3-Butanediol Chemical compound CC(O)CCO PUPZLCDOIYMWBV-UHFFFAOYSA-N 0.000 description 2
- UNMJLQGKEDTEKJ-UHFFFAOYSA-N (3-ethyloxetan-3-yl)methanol Chemical compound CCC1(CO)COC1 UNMJLQGKEDTEKJ-UHFFFAOYSA-N 0.000 description 2
- 125000003903 2-propenyl group Chemical group [H]C([*])([H])C([H])=C([H])[H] 0.000 description 2
- KAKZBPTYRLMSJV-UHFFFAOYSA-N Butadiene Chemical compound C=CC=C KAKZBPTYRLMSJV-UHFFFAOYSA-N 0.000 description 2
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- 239000006087 Silane Coupling Agent Substances 0.000 description 2
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- 239000011324 bead Substances 0.000 description 1
- 230000008901 benefit Effects 0.000 description 1
- 125000001797 benzyl group Chemical group [H]C1=C([H])C([H])=C(C([H])=C1[H])C([H])([H])* 0.000 description 1
- 230000000903 blocking effect Effects 0.000 description 1
- 125000006226 butoxyethyl group Chemical group 0.000 description 1
- 125000000484 butyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- 238000011088 calibration curve Methods 0.000 description 1
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- 229920002678 cellulose Polymers 0.000 description 1
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- 239000003086 colorant Substances 0.000 description 1
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- 239000011231 conductive filler Substances 0.000 description 1
- 229930003836 cresol Natural products 0.000 description 1
- 238000005520 cutting process Methods 0.000 description 1
- FOTKYAAJKYLFFN-UHFFFAOYSA-N decane-1,10-diol Chemical compound OCCCCCCCCCCO FOTKYAAJKYLFFN-UHFFFAOYSA-N 0.000 description 1
- 125000002704 decyl group Chemical group [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])* 0.000 description 1
- 239000012954 diazonium Substances 0.000 description 1
- 150000001989 diazonium salts Chemical class 0.000 description 1
- GGSUCNLOZRCGPQ-UHFFFAOYSA-N diethylaniline Chemical class CCN(CC)C1=CC=CC=C1 GGSUCNLOZRCGPQ-UHFFFAOYSA-N 0.000 description 1
- ZUOUZKKEUPVFJK-UHFFFAOYSA-N diphenyl Chemical group C1=CC=CC=C1C1=CC=CC=C1 ZUOUZKKEUPVFJK-UHFFFAOYSA-N 0.000 description 1
- VFHVQBAGLAREND-UHFFFAOYSA-N diphenylphosphoryl-(2,4,6-trimethylphenyl)methanone Chemical class CC1=CC(C)=CC(C)=C1C(=O)P(=O)(C=1C=CC=CC=1)C1=CC=CC=C1 VFHVQBAGLAREND-UHFFFAOYSA-N 0.000 description 1
- SZXQTJUDPRGNJN-UHFFFAOYSA-N dipropylene glycol Chemical compound OCCCOCCCO SZXQTJUDPRGNJN-UHFFFAOYSA-N 0.000 description 1
- 230000005684 electric field Effects 0.000 description 1
- 150000002148 esters Chemical class 0.000 description 1
- 125000001495 ethyl group Chemical group [H]C([H])([H])C([H])([H])* 0.000 description 1
- RBVLUTAXWVILBT-UHFFFAOYSA-N ethyl prop-2-eneperoxoate Chemical compound CCOOC(=O)C=C RBVLUTAXWVILBT-UHFFFAOYSA-N 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 239000003063 flame retardant Substances 0.000 description 1
- 229920002457 flexible plastic Polymers 0.000 description 1
- 230000009969 flowable effect Effects 0.000 description 1
- 125000003983 fluorenyl group Chemical group C1(=CC=CC=2C3=CC=CC=C3CC12)* 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- 230000014509 gene expression Effects 0.000 description 1
- 235000011187 glycerol Nutrition 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 125000003187 heptyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- XXMIOPMDWAUFGU-UHFFFAOYSA-N hexane-1,6-diol Chemical compound OCCCCCCO XXMIOPMDWAUFGU-UHFFFAOYSA-N 0.000 description 1
- FUZZWVXGSFPDMH-UHFFFAOYSA-N hexanoic acid Chemical compound CCCCCC(O)=O FUZZWVXGSFPDMH-UHFFFAOYSA-N 0.000 description 1
- 125000004051 hexyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 description 1
- XMBWDFGMSWQBCA-UHFFFAOYSA-N hydrogen iodide Chemical class I XMBWDFGMSWQBCA-UHFFFAOYSA-N 0.000 description 1
- 125000002883 imidazolyl group Chemical group 0.000 description 1
- 229910052738 indium Inorganic materials 0.000 description 1
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 1
- 239000003112 inhibitor Substances 0.000 description 1
- 239000003999 initiator Substances 0.000 description 1
- 238000007689 inspection Methods 0.000 description 1
- 239000011810 insulating material Substances 0.000 description 1
- 238000009413 insulation Methods 0.000 description 1
- 229910052741 iridium Inorganic materials 0.000 description 1
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 1
- 125000000959 isobutyl group Chemical group [H]C([H])([H])C([H])(C([H])([H])[H])C([H])([H])* 0.000 description 1
- 125000001972 isopentyl group Chemical group [H]C([H])([H])C([H])(C([H])([H])[H])C([H])([H])C([H])([H])* 0.000 description 1
- 238000003475 lamination Methods 0.000 description 1
- 239000011159 matrix material Substances 0.000 description 1
- 238000000691 measurement method Methods 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 125000000956 methoxy group Chemical group [H]C([H])([H])O* 0.000 description 1
- 229910052750 molybdenum Inorganic materials 0.000 description 1
- 239000011733 molybdenum Substances 0.000 description 1
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 description 1
- SLCVBVWXLSEKPL-UHFFFAOYSA-N neopentyl glycol Chemical compound OCC(C)(C)CO SLCVBVWXLSEKPL-UHFFFAOYSA-N 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 150000004767 nitrides Chemical class 0.000 description 1
- 125000001400 nonyl 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])[H] 0.000 description 1
- OTLDLKLSNZMTTA-UHFFFAOYSA-N octahydro-1h-4,7-methanoindene-1,5-diyldimethanol Chemical compound C1C2C3C(CO)CCC3C1C(CO)C2 OTLDLKLSNZMTTA-UHFFFAOYSA-N 0.000 description 1
- 229910052762 osmium Inorganic materials 0.000 description 1
- SYQBFIAQOQZEGI-UHFFFAOYSA-N osmium atom Chemical compound [Os] SYQBFIAQOQZEGI-UHFFFAOYSA-N 0.000 description 1
- 150000002921 oxetanes Chemical class 0.000 description 1
- NFHFRUOZVGFOOS-UHFFFAOYSA-N palladium;triphenylphosphane Chemical compound [Pd].C1=CC=CC=C1P(C=1C=CC=CC=1)C1=CC=CC=C1.C1=CC=CC=C1P(C=1C=CC=CC=1)C1=CC=CC=C1.C1=CC=CC=C1P(C=1C=CC=CC=1)C1=CC=CC=C1.C1=CC=CC=C1P(C=1C=CC=CC=1)C1=CC=CC=C1 NFHFRUOZVGFOOS-UHFFFAOYSA-N 0.000 description 1
- 230000002093 peripheral effect Effects 0.000 description 1
- 150000004714 phosphonium salts Chemical class 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 229920003207 poly(ethylene-2,6-naphthalate) Polymers 0.000 description 1
- 229920000058 polyacrylate Polymers 0.000 description 1
- 229920006122 polyamide resin Polymers 0.000 description 1
- 229920000728 polyester Polymers 0.000 description 1
- 229920001225 polyester resin Polymers 0.000 description 1
- 239000004645 polyester resin Substances 0.000 description 1
- 239000011112 polyethylene naphthalate Substances 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 229920000098 polyolefin Polymers 0.000 description 1
- 229920000069 polyphenylene sulfide Polymers 0.000 description 1
- 229920001155 polypropylene Polymers 0.000 description 1
- 229920005749 polyurethane resin Polymers 0.000 description 1
- 239000004800 polyvinyl chloride Substances 0.000 description 1
- 229920000915 polyvinyl chloride Polymers 0.000 description 1
- 229920000131 polyvinylidene Polymers 0.000 description 1
- 239000005033 polyvinylidene chloride Substances 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 229940090181 propyl acetate Drugs 0.000 description 1
- 125000001436 propyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- 229910052703 rhodium Inorganic materials 0.000 description 1
- 239000010948 rhodium Substances 0.000 description 1
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 238000001878 scanning electron micrograph Methods 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 229910000077 silane Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 239000010944 silver (metal) Substances 0.000 description 1
- 229910000679 solder Inorganic materials 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
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- 150000003440 styrenes Chemical class 0.000 description 1
- 125000005504 styryl group Chemical group 0.000 description 1
- 150000003890 succinate salts Chemical class 0.000 description 1
- 239000002344 surface layer Substances 0.000 description 1
- 229920003051 synthetic elastomer Polymers 0.000 description 1
- 239000005061 synthetic rubber Substances 0.000 description 1
- KKEYFWRCBNTPAC-UHFFFAOYSA-L terephthalate(2-) Chemical compound [O-]C(=O)C1=CC=C(C([O-])=O)C=C1 KKEYFWRCBNTPAC-UHFFFAOYSA-L 0.000 description 1
- 125000000999 tert-butyl group Chemical group [H]C([H])([H])C(*)(C([H])([H])[H])C([H])([H])[H] 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- UWHCKJMYHZGTIT-UHFFFAOYSA-N tetraethylene glycol Chemical compound OCCOCCOCCOCCO UWHCKJMYHZGTIT-UHFFFAOYSA-N 0.000 description 1
- 229920002803 thermoplastic polyurethane Polymers 0.000 description 1
- 125000003396 thiol group Chemical group [H]S* 0.000 description 1
- 239000013008 thixotropic agent Substances 0.000 description 1
- 229910052718 tin Inorganic materials 0.000 description 1
- 239000011135 tin Substances 0.000 description 1
- ZIBGPFATKBEMQZ-UHFFFAOYSA-N triethylene glycol Chemical compound OCCOCCOCCO ZIBGPFATKBEMQZ-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
- 238000009281 ultraviolet germicidal irradiation Methods 0.000 description 1
- NQPDZGIKBAWPEJ-UHFFFAOYSA-N valeric acid Chemical compound CCCCC(O)=O NQPDZGIKBAWPEJ-UHFFFAOYSA-N 0.000 description 1
- 229920001567 vinyl ester resin Polymers 0.000 description 1
- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 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
- 239000011787 zinc oxide Substances 0.000 description 1
Images
Classifications
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J9/00—Adhesives characterised by their physical nature or the effects produced, e.g. glue sticks
- C09J9/02—Electrically-conducting adhesives
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/34—Silicon-containing compounds
- C08K3/36—Silica
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J11/00—Features of adhesives not provided for in group C09J9/00, e.g. additives
- C09J11/02—Non-macromolecular additives
- C09J11/04—Non-macromolecular additives inorganic
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J201/00—Adhesives based on unspecified macromolecular compounds
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J7/00—Adhesives in the form of films or foils
- C09J7/30—Adhesives in the form of films or foils characterised by the adhesive composition
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
- H01B5/00—Non-insulated conductors or conductive bodies characterised by their form
- H01B5/16—Non-insulated conductors or conductive bodies characterised by their form comprising conductive material in insulating or poorly conductive material, e.g. conductive rubber
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
- H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
- H01L21/04—Manufacture or treatment of semiconductor devices or of parts thereof the devices having potential barriers, e.g. a PN junction, depletion layer or carrier concentration layer
- H01L21/50—Assembly of semiconductor devices using processes or apparatus not provided for in a single one of the subgroups H01L21/06 - H01L21/326, e.g. sealing of a cap to a base of a container
- H01L21/60—Attaching or detaching leads or other conductive members, to be used for carrying current to or from the device in operation
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
- H05K3/00—Apparatus or processes for manufacturing printed circuits
- H05K3/30—Assembling printed circuits with electric components, e.g. with resistor
- H05K3/32—Assembling printed circuits with electric components, e.g. with resistor electrically connecting electric components or wires to printed circuits
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K2201/00—Specific properties of additives
- C08K2201/002—Physical properties
- C08K2201/003—Additives being defined by their diameter
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J2301/00—Additional features of adhesives in the form of films or foils
- C09J2301/20—Additional features of adhesives in the form of films or foils characterized by the structural features of the adhesive itself
- C09J2301/208—Additional features of adhesives in the form of films or foils characterized by the structural features of the adhesive itself the adhesive layer being constituted by at least two or more adjacent or superposed adhesive layers, e.g. multilayer adhesive
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J2301/00—Additional features of adhesives in the form of films or foils
- C09J2301/20—Additional features of adhesives in the form of films or foils characterized by the structural features of the adhesive itself
- C09J2301/21—Additional features of adhesives in the form of films or foils characterized by the structural features of the adhesive itself the adhesive layer being formed by alternating adhesive areas of different nature
Definitions
- the present disclosure relates to an adhesive film for circuit connection, an inorganic filler-containing composition, a circuit connection structure, and a method for manufacturing the same.
- a glass substrate is used as a substrate, and as a circuit material formed on the glass substrate, a metal such as aluminum is used for the circuit of the base layer, and ITO (Indium Tin Oxide) or the like is used for the electrode of the surface layer.
- a metal such as aluminum
- ITO Indium Tin Oxide
- a flexible plastic substrate such as a polyimide substrate is used as the substrate, and plastic is used. It is becoming mainstream that Ti is used as a circuit material formed on a substrate.
- a pressure-sensitive adhesive layer and a flexible member such as a polyethylene terephthalate (PET) substrate are usually arranged for the purpose of imparting flexibility (see, for example, Patent Document 1).
- COG chip on glass
- various electronic components such as drive ICs are mounted directly on the glass substrate of a display panel from the viewpoint of fine pitch, light weight and thinness.
- COG mounting method for example, a circuit connection is made by thermocompression bonding a liquid crystal drive IC onto a glass substrate via a circuit connection adhesive film having anisotropic conductivity in which conductive particles are dispersed in an adhesive. A method of obtaining a structure is used.
- the low pressure mounting has an advantage that the selectivity of the connecting member and the peripheral member can be enhanced. For example, it can be expected that the connection structure will be made thinner by being able to be mounted on a thinned glass substrate.
- the mounting body manufactured under such a low pressure condition tends to have a high connection resistance between the opposing electrodes, and it tends to be difficult to obtain sufficient conduction characteristics. Therefore, the present inventors have studied to enhance the fluidity of the adhesive existing between the conductive particles and the electrode during thermocompression bonding of the adhesive film.
- an adhesive with high flow rate it is considered effective to add an inorganic filler such as a silica filler having a relatively large primary particle size.
- an inorganic filler such as a silica filler having a relatively large primary particle size.
- it has been clarified that the addition of a normally available silica filler may cause a problem of defect determination in an automatic visual inspection apparatus. In order to improve production efficiency, it is desirable to reduce the occurrence of defect judgment.
- one aspect of the present disclosure is an adhesive film for circuit connection containing conductive particles, and the adhesive film includes a region A containing an inorganic filler in the thickness direction of the film.
- the particle size D50 at the time of 50% accumulation is 0.5 to 1.0 ⁇ m and the particle size D95 at the time of 95% accumulation is 0.9 to 2.0 ⁇ m in the volume-based particle size distribution.
- an adhesive film for circuit connection formed from a thermosetting composition containing.
- the region A contains the inorganic filler having the specific particle size distribution, thereby limiting the inclusion of the inorganic filler that causes a large indentation in the film. It is possible to secure high fluidity, and even when the circuit members are connected to each other at low pressure, sufficient continuity can be ensured between the opposing electrodes of the circuit connection structure, and defects due to the automatic visual inspection device are obtained. It is possible to sufficiently suppress the generation of large indentations that are a factor in the determination.
- the circuit connection adhesive film on the side surface may include a region S containing no conductive particles in the thickness direction of the film, and the region A may be provided in at least a part of the region S. In this case, it becomes easy to prevent bridging by conductive particles between the circuit electrodes of the adherend (for example, the circuit member) in contact with the region A side of the adhesive film.
- the inorganic filler may be a silica filler.
- a circuit comprising an inorganic filler-containing composition containing an inorganic filler having an hourly particle size D50 of 0.5 to 1.0 ⁇ m and a 95% cumulative particle size D95 of 0.9 to 2.0 ⁇ m.
- an adhesive film for connection is provided.
- the adhesive film for circuit connection on the other side surface even when the circuit members are connected to each other at low pressure, the conduction between the facing electrodes of the circuit connection structure can be sufficiently ensured, and the automatic appearance can be obtained. It is possible to sufficiently suppress the generation of large indentations, which is a factor in determining defects by the inspection device. Further, according to this adhesive film for circuit connection, the flow of conductive particles at the time of circuit connection can be suppressed by the photocured material, so that the conductive particles can be efficiently captured on the electrode, and high connection reliability is achieved. It will be easier to obtain.
- the inorganic filler may be a silica filler.
- the circuit-connecting adhesive film on the other side thereof is a third adhesive containing a third thermosetting resin component laminated on the side opposite to the second adhesive layer of the first adhesive layer.
- a further agent layer may be provided.
- the adhesive film for circuit connection on the other side thereof can easily secure the transferability and the characteristics in various reliability tests, and can easily improve the margin of the product.
- compositions used to form an inorganic filler-containing region in a circuit connecting member containing conductive particles and an inorganic filler which is a 50% cumulative grain in a volume-based particle size distribution.
- an inorganic filler-containing composition containing an inorganic filler having a diameter D50 of 0.5 to 1.0 ⁇ m and a particle size D95 at a time of 95% accumulation of 0.9 to 2.0 ⁇ m.
- the composition containing the inorganic filler on the other side surface the region A in the circuit connection adhesive film on the one side surface, the second adhesive layer in the circuit connection adhesive film on the other side surface, and the like.
- An inorganic filler-containing region can be formed.
- the composition containing the inorganic filler on the other side thereof is less likely to cause poor coating even when a thin layer is formed by coating, and the coating yield can be increased.
- the inorganic filler-containing layer formed by the inorganic filler-containing composition on the other side thereof may have sufficiently few appearance defects such as scratches.
- the inorganic filler may be a silica filler.
- the inorganic filler-containing composition on the other side thereof can further contain a thermoplastic resin.
- the inorganic filler-containing composition on the other side can be used to form an adhesive layer having a thickness of 10 ⁇ m or less.
- Another aspect of the present disclosure is to interpose the above-mentioned circuit connection adhesive film between the first circuit member having the first electrode and the second circuit member having the second electrode.
- a method for manufacturing a circuit connection structure including a step of thermally crimping a circuit member 1 and a second circuit member to electrically connect the first electrode and the second electrode to each other.
- one of the first circuit member and the second circuit member may be an IC chip, and the other may be a plastic substrate having an electrode containing Ti. ..
- Another aspect of the present disclosure is disposed between a first circuit member having a first electrode, a second circuit member having a second electrode, and a first circuit member and a second circuit member.
- one of the first circuit member and the second circuit member may be an IC chip, and the other may be a plastic substrate having an electrode containing Ti.
- the present disclosure even when the circuit members are connected to each other at a low pressure, sufficient continuity can be ensured between the facing electrodes of the circuit connection structure, and it becomes a factor of defect determination by the automatic visual inspection device. It is possible to provide an adhesive film for circuit connection capable of sufficiently suppressing the generation of large indentations and an inorganic filler-containing composition suitable for producing such a member for circuit connection. Further, according to the present disclosure, it is possible to provide a method for manufacturing a circuit connection structure and a circuit connection structure using the above-mentioned adhesive film for circuit connection.
- FIG. 1 is a schematic cross-sectional view showing an embodiment of an adhesive film for circuit connection.
- FIG. 2 is a schematic cross-sectional view showing a method of manufacturing an adhesive film for circuit connection.
- FIG. 3 is a schematic cross-sectional view showing an embodiment of a circuit connection structure.
- FIG. 4 is a schematic cross-sectional view showing an embodiment of a manufacturing process of a circuit connection structure.
- the numerical range indicated by using "-" indicates a range including the numerical values before and after "-" as the minimum value and the maximum value, respectively.
- the upper limit value or the lower limit value of the numerical range of one step may be replaced with the upper limit value or the lower limit value of the numerical range of another step.
- the upper limit value or the lower limit value of the numerical range may be replaced with the value shown in the examples.
- the upper limit value and the lower limit value described individually can be arbitrarily combined.
- the term "(meth) acrylate” means at least one of acrylate and the corresponding methacrylate.
- each component in the composition means the total amount of the plurality of substances present in the composition when a plurality of substances corresponding to each component are present in the composition, unless otherwise specified.
- the circuit connection adhesive film of the present embodiment contains conductive particles and contains a region A containing an inorganic filler in the thickness direction of the film, and the region A is a particle at 50% accumulation in the volume-based particle size distribution.
- the thermosetting composition forming the region A can contain a polymerizable compound and a thermal polymerization initiator.
- the circuit connection adhesive film of the present embodiment includes a region S that does not contain conductive particles in the thickness direction of the film, and the region A may be provided in at least a part of the region S.
- the ratio of the region A in the region S is 60% or more, 80% or more, or 100% with respect to the range in the thickness direction of the film from the viewpoint of facilitating the continuity between the facing electrodes even in low-voltage mounting. There may be.
- the circuit connection adhesive film of the present embodiment contains a region P further containing a cured product of a photocurable resin component in the thickness direction of the film, and conductive particles may be dispersed in the region P.
- FIG. 1 is a schematic cross-sectional view showing an embodiment of the adhesive film for circuit connection of the present embodiment.
- the circuit connection adhesive film 1a (hereinafter, may be simply referred to as “adhesive film 1a”) shown in FIG. 1 (a) includes the conductive particles 4, the cured product of the photocurable resin component, and ( A first adhesive layer 2 containing an adhesive component 5 containing a first) thermocurable resin component, and a (second) thermocurable resin component provided on the first adhesive layer 2.
- a second adhesive layer 3 containing the above-mentioned material is provided.
- the circuit connection adhesive film 1b (hereinafter, may be simply referred to as “adhesive film 1b”) shown in FIG. 1 (b) is the second adhesive layer of the first adhesive layer 2. It has the same structure as the adhesive film 1a except that a third adhesive layer containing a (third) thermosetting resin component is laminated on the opposite side to the third.
- circuit connection adhesive film of the present embodiment will be described with reference to FIG.
- the adhesive films 1a and 1b the conductive particles 4 are dispersed in the first adhesive layer 2. Therefore, the adhesive films 1a and 1b can be a circuit-connecting adhesive film (anisotropic adhesive film) having anisotropic conductivity.
- the adhesive films 1a and 1b are interposed between the first circuit member having the first electrode and the second circuit member having the second electrode, and the first circuit member and the second circuit member are interposed. May be used to electrically connect the first electrode and the second electrode to each other by thermocompression bonding.
- the first adhesive layer 2 is a curing of conductive particles 4 (hereinafter, may be referred to as "(A) component”) and a photocurable resin component (hereinafter, may be referred to as “(B) component”). It contains a substance and a thermosetting resin component (hereinafter, may be referred to as "(C) component”).
- a composition layer composed of a composition containing the component (A), the component (B), and the component (C) is irradiated with light energy, and the component (B) is subjected to light energy. It can be obtained by polymerizing the contained components and curing the component (B).
- the first adhesive layer 2 contains the component (A), the cured product of the component (B), and the adhesive component 5 containing the component (C).
- the cured product of the component (B) may be a cured product obtained by completely curing the component (B), or may be a cured product obtained by curing a part of the component (B).
- the component (C) is a component that can flow when connected to a circuit, and is, for example, an uncured curable resin component.
- Component (A) Conductive particles
- the component (A) is not particularly limited as long as it is a particle having conductivity, and is a metal particle composed of a metal such as Au, Ag, Pd, Ni, Cu, or solder, or conductive carbon. It may be conductive carbon particles composed of.
- the component (A) may be a coated conductive particle containing a nucleus containing non-conductive glass, ceramic, plastic (polystyrene, etc.) and the like, and a coating layer containing the metal or conductive carbon and covering the nucleus. good.
- the component (A) preferably contains metal particles formed of a heat-meltable metal or a core containing plastic, and contains a metal or conductive carbon and has a coating layer covering the core.
- Such coated conductive particles can easily deform the cured product of the thermosetting resin component by heating or pressurizing, when the electrodes are electrically connected to each other, the electrode and the component (A) are connected to each other.
- the contact area can be increased and the conductivity between the electrodes can be further improved.
- conductive particles those having palladium plating can be used from the viewpoint of facilitating the development of low resistance to the circuit having the Ti surface.
- palladium plating can be provided on the outermost surface of the conductive particles.
- conductive particles in which the surface of the plastic core is Ni-plated and the outermost surface is substituted-plated with Pd can be used, and such conductive particles can be used from the viewpoint of preventing short circuits between the conductive particles.
- Those in which insulating fine particles are supported on the surface thereof may be used.
- a ceramic core material having a diameter of 100 nm to 200 nm is incorporated into the plating, and then Pd plating is performed to support insulating fine particles as necessary. May be good.
- the component (A) may be an insulating coated conductive particle containing the above-mentioned metal particles, conductive carbon particles, or coated conductive particles and an insulating material such as a resin and having an insulating layer covering the surface of the particles. good.
- the component (A) is an insulating coated conductive particle, even when the content of the component (A) is large, the insulating layer is provided on the surface of the particle, so that the component (A) is short-circuited due to contact with each other. The generation can be suppressed, and the insulation between adjacent electrode circuits can be improved.
- one of the above-mentioned various conductive particles may be used alone or in combination of two or more.
- the maximum particle size of the component (A) needs to be smaller than the minimum distance between the electrodes (the shortest distance between adjacent electrodes).
- the maximum particle size of the component (A) may be 1.0 ⁇ m or more, 2.0 ⁇ m or more, or 2.5 ⁇ m or more from the viewpoint of excellent dispersibility and conductivity.
- the maximum particle size of the component (A) may be 20 ⁇ m or less, 10 ⁇ m or less, or 5 ⁇ m or less from the viewpoint of excellent dispersibility and conductivity.
- the particle size of any 300 conductive particles (pcs) is measured by observation using a scanning electron microscope (SEM), and the largest value obtained is the maximum particle size of the component (A).
- SEM scanning electron microscope
- the particle size of the component (A) is the diameter of a circle circumscribing the conductive particles in the SEM image.
- the average particle size of the component (A) may be 1.0 ⁇ m or more, 2.0 ⁇ m or more, or 2.5 ⁇ m or more from the viewpoint of excellent dispersibility and conductivity.
- the average particle size of the component (A) may be 20 ⁇ m or less, 10 ⁇ m or less, or 5 ⁇ m or less from the viewpoint of excellent dispersibility and conductivity.
- the particle size of any 300 conductive particles (pcs) is measured by observation using a scanning electron microscope (SEM), and the average value of the obtained particle sizes is taken as the average particle size.
- the component (A) is preferably uniformly dispersed.
- the particle density of the component (A) in the adhesive films 1a and 1b is 100 / mm 2 or more, 1000 / mm 2 or more, 3000 / mm 2 or more, or 5000 from the viewpoint of obtaining stable connection resistance. It may be / mm 2 or more.
- the particle density of the component (A) in the adhesive films 1a and 1b is 100,000 pieces / mm 2 or less, 70,000 pieces / mm 2 or less, 50,000 pieces / mm 2 or less, from the viewpoint of improving the insulating property between adjacent electrodes. Alternatively, it may be 30,000 pieces / mm 2 or less.
- the content of the component (A) is 1% by mass or more, 5% by mass or more, or 10% by mass or more based on the total mass of the first adhesive layer from the viewpoint of further improving the conductivity. It may be there.
- the content of the component (A) may be 60% by mass or less, 50% by mass or less, or 40% by mass or less based on the total mass of the first adhesive layer from the viewpoint of easily suppressing a short circuit.
- the effect of the present invention tends to be remarkably exhibited.
- the content of the component (A) in the composition or the composition layer (based on the total mass of the composition or the composition layer) may be the same as the above range.
- Component (B) Photocurable resin component
- the component (B) is not particularly limited as long as it is a resin component that is cured by light irradiation, but may be a resin component having radical curability from the viewpoint of better connection resistance. ..
- the component (B) contains, for example, a radically polymerizable compound (hereinafter, may be referred to as “(B1) component”) and a photoradical polymerization initiator (hereinafter, may be referred to as “(B2) component”). You may be.
- the component (B) can be a component composed of the component (B1) and the component (B2).
- Component (B1) Radical Polymerizable Compound
- the component (B1) is a compound polymerized by radicals generated from the component (B2) by irradiation with light (for example, ultraviolet light).
- the component (B1) may be either a monomer or a polymer (or oligomer) obtained by polymerizing one or more kinds of monomers.
- the component (B1) may be used alone or in combination of two or more.
- the component (B1) is a compound having a radically polymerizable group that reacts with a radical.
- the radically polymerizable group include a (meth) acryloyl group, a vinyl group, an allyl group, a styryl group, an alkenyl group, an alkenylene group, a maleimide group and the like.
- the number of radically polymerizable groups (number of functional groups) of the component (B1) is 2 or more from the viewpoint that the desired melt viscosity can be easily obtained after polymerization, the effect of reducing the connection resistance is further improved, and the connection reliability is superior. It may be 10 or less from the viewpoint of suppressing curing shrinkage during polymerization. Further, in order to balance the crosslink density and the curing shrinkage, in addition to the compound having the number of radically polymerizable groups within the above range, a compound having the number of radically polymerizable groups outside the above range may be used. good.
- the component (B1) may contain, for example, a polyfunctional (bifunctional or higher) (meth) acrylate from the viewpoint of suppressing the flow of conductive particles.
- the polyfunctional (bifunctional or higher) (meth) acrylate may be a bifunctional (meth) acrylate, and the bifunctional (meth) acrylate may be a bifunctional aromatic (meth) acrylate.
- polyfunctional (meth) acrylate examples include ethylene glycol di (meth) acrylate, diethylene glycol di (meth) acrylate, triethylene glycol di (meth) acrylate, tetraethylene glycol di (meth) acrylate, and polyethylene glycol di (meth) acrylate.
- the content of the polyfunctional (bifunctional or higher) (meth) acrylate is, for example, 40 to 100, based on the total mass of the component (B1), from the viewpoint of achieving both the effect of reducing the connection resistance and the suppression of particle flow. It may be% by mass, 50 to 100% by mass, or 60 to 100% by mass.
- the component (B1) may further contain a monofunctional (meth) acrylate in addition to the polyfunctional (bifunctional or higher) (meth) acrylate.
- a monofunctional (meth) acrylate examples include (meth) acrylic acid; methyl (meth) acrylate, ethyl (meth) acrylate, butyl (meth) acrylate, isobutyl (meth) acrylate, and tert-butyl (meth) acrylate.
- (Meta) acrylates having an alicyclic epoxy group such as, ( Examples thereof include (meth) acrylate having an oxetanyl group such as 3-ethyloxetane-3-yl) methyl (meth) acrylate.
- the content of the monofunctional (meth) acrylate may be, for example, 0 to 60% by mass, 0 to 50% by mass, or 0 to 40% by mass based on the total mass of the component (B1).
- the cured product of the component (B) may have, for example, a polymerizable group that reacts with a substance other than a radical.
- the polymerizable group that reacts with a non-radical substance may be, for example, a cationically polymerizable group that reacts with a cation.
- the cationically polymerizable group include an epoxy group such as a glycidyl group, an alicyclic epoxy group such as an epoxycyclohexylmethyl group, and an oxetanyl group such as an ethyloxetanylmethyl group.
- the cured product of the component (B) having a polymerizable group that reacts by other than radicals is, for example, a (meth) acrylate having an epoxy group, a (meth) acrylate having an alicyclic epoxy group, and a (meth) acrylate having an oxetanyl group. It can be introduced by using a (meth) acrylate having a polymerizable group that reacts with a non-radical substance such as (B) as a component (B).
- (B1) Mass ratio of (meth) acrylate having a polymerizable group that reacts with other than radicals to the total mass of the component (mass of (meth) acrylate having a polymerizable group that reacts with other than radicals (charged amount) / (B1)
- the total mass (charged amount) of the components may be, for example, 0 to 0.7, 0 to 0.5, or 0 to 0.3 from the viewpoint of improving reliability.
- the component (B1) may contain other radically polymerizable compounds in addition to polyfunctional (bifunctional or higher) and monofunctional (meth) acrylates.
- examples of other radically polymerizable compounds include maleimide compounds, vinyl ether compounds, allyl compounds, styrene derivatives, acrylamide derivatives, nadiimide derivatives and the like.
- the content of the other radically polymerizable compound may be, for example, 0 to 40% by mass based on the total mass of the component (B1).
- Component (B2) Photoradical Polymerization Initiator
- the component (B2) comprises light containing a wavelength in the range of 150 to 750 nm, preferably light containing a wavelength in the range of 254 to 405 nm, and more preferably a wavelength in the range of 365 nm. It is a photopolymerization initiator that generates radicals by irradiation with light (for example, ultraviolet light).
- the component (B2) one type may be used alone, or a plurality of them may be used in combination.
- the component (B2) is decomposed by light to generate free radicals. That is, the component (B2) is a compound that generates radicals by applying light energy from the outside.
- the component (B2) includes an oxime ester structure, a bisimidazole structure, an acridine structure, an ⁇ -aminoalkylphenone structure, an aminobenzophenone structure, an N-phenylglycine structure, an acylphosphine oxide structure, a benzyldimethylketal structure, and an ⁇ -hydroxyalkylphenone structure. It may be a compound having a structure such as. As the component (B2), one type may be used alone, or a plurality of them may be used in combination.
- the component (B2) is selected from the group consisting of an oxime ester structure, an ⁇ -aminoalkylphenone structure, and an acylphosphine oxide structure from the viewpoint that the desired melt viscosity can be easily obtained and the effect of reducing the connection resistance is superior. It may be a compound having at least one structure.
- the compound having an oxime ester structure examples include 1-phenyl-1,2-butandion-2- (o-methoxycarbonyl) oxime and 1-phenyl-1,2-propanedione-2- (o-methoxycarbonyl).
- the compound having an ⁇ -aminoalkylphenone structure include 2-methyl-1- [4- (methylthio) phenyl] -2-morpholinopropane-1-one and 2-benzyl-2-dimethylamino-1. -Morphorinophenyl) -butanone-1 and the like.
- the compound having an acylphosphine oxide structure include bis (2,6-dimethoxybenzoyl) -2,4,4-trimethyl-pentylphosphine oxide and bis (2,4,6, -trimethylbenzoyl) -phenylphosphine.
- examples thereof include oxides, 2,4,6-trimethylbenzoyl-diphenylphosphine oxides and the like.
- the content of the component (B2) is, for example, 0.1 to 10 parts by mass, 0.3 to 7 parts by mass, or 0 with respect to 100 parts by mass of the component (B1) from the viewpoint of suppressing the flow of conductive particles. It may be 5 to 5 parts by mass.
- the content of the cured product of the component (B) is 1% by mass or more, 5% by mass or more, or 10% by mass or more, based on the total mass of the first adhesive layer, from the viewpoint of suppressing the flow of conductive particles. May be.
- the content of the cured product of the component (B) is 50% by mass or less, 40% by mass or less, or 30% by mass based on the total mass of the first adhesive layer from the viewpoint of developing low resistance in low-pressure mounting. It may be as follows.
- the content of the component (B) in the composition or the composition layer for forming the first adhesive layer (based on the total mass of the composition or the composition layer) may be the same as the above range.
- Thermosetting resin component is, for example, a cationically polymerizable compound (hereinafter, may be referred to as “(C1) component”) and a thermally cationic polymerization initiator (hereinafter, “(C2)). It may be referred to as "ingredient").
- the component (C) can be a component composed of the component (C1) and the component (C2).
- the first thermosetting resin component and the second thermosetting resin component mean the thermosetting resin components contained in the first adhesive layer and the second adhesive layer, respectively.
- the types, combinations, and contents of the first thermosetting resin component and the components contained in the second thermosetting resin component are the same as each other. May be different.
- Component (C1) Cationicly polymerizable compound
- the component (C1) is a compound that crosslinks by reacting with the component (C2) by heat.
- the component (C1) means a compound having no radically polymerizable group that reacts with a radical, and the component (C1) is not included in the component (B1).
- the component (C1) may be a compound having one or more ring-opening polymerizable cyclic ether groups in the molecule from the viewpoint of further improving the effect of reducing the connection resistance and improving the connection reliability.
- the component (C1) may be used alone or in combination of two or more.
- the compound having one or more ring-opening polymerizable cyclic ether groups in the molecule may be, for example, at least one selected from the group consisting of an oxetane compound and an alicyclic epoxy compound.
- the component (C1) preferably contains at least one oxetane compound and at least one alicyclic epoxy compound from the viewpoint that the desired melt viscosity can be easily obtained.
- the oxetane compound as the component (C1) can be used without particular limitation as long as it is a compound having an oxetane group and no radically polymerizable group.
- Commercially available oxetane compounds include, for example, ETERNCOLL OXBP (trade name, manufactured by Ube Industries, Ltd.), OXSQ, OXT-121, OXT-221, OXT-101, OXT-212 (trade name, manufactured by Toagosei Co., Ltd.). And so on. These may use one kind of compound alone or may use a plurality of compounds in combination.
- the alicyclic epoxy compound as the component (C1) can be used without particular limitation as long as it is a compound having an alicyclic epoxy group (for example, an epoxycyclohexyl group) and no radical polymerizable group.
- Examples of commercially available alicyclic epoxy compounds include EHPE3150, EHPE3150CE, seroxide 8010, seroxide 2021P, and seroxide 2081 (trade name, manufactured by Daicel Corporation). These may use one kind of compound alone or may use a plurality of compounds in combination.
- Component (C2) Thermal Cationic Polymerization Initiator
- the component (C2) is a thermal polymerization initiator that generates an acid or the like by heating to initiate polymerization.
- the component (C2) may be a salt compound composed of a cation and an anion.
- the component (C2) is, for example, BF 4- , BR 4- ( R indicates a phenyl group substituted with 2 or more fluorine atoms or 2 or more trifluoromethyl groups) , PF 6- , SbF 6- . , AsF 6 ⁇ and the like, sulfonium salt, phosphonium salt, ammonium salt, diazonium salt, iodonium salt, onium salt such as anilinium salt and the like. These may be used individually by 1 type, and may be used in combination of a plurality of types.
- the component (C2) is, for example, an anion containing boron as a constituent element, that is, BF 4- or BR 4- ( R is two or more fluorine atoms or two or more trifluoromethyl groups. It may be a salt compound having a substituted phenyl group.).
- the anion containing boron as a constituent element may be BR 4- , and more specifically, tetrakis (pentafluorophenyl) borate.
- the onium salt as the component (C2) may be, for example, an anilinium salt because it has resistance to a substance that can inhibit curing against cationic curing.
- anilinium salt compound examples include N, N-dialkylanilinium salts such as N, N-dimethylanilinium salt and N, N-diethylanilinium salt.
- the component (C2) may be an anilinium salt having an anion containing boron as a constituent element.
- anilinium salt compounds include CXC-1821 (trade name, manufactured by King Industries) and the like.
- the content of the component (C2) is, for example, 0 with respect to 100 parts by mass of the component (C1) from the viewpoint of ensuring the formability and curability of the adhesive film for forming the first adhesive layer. It may be 1 to 25 parts by mass, 1 to 20 parts by mass, 3 to 18 parts by mass, or 5 to 15 parts by mass.
- the content of the component (C) is 5% by mass or more based on the total mass of the first adhesive layer from the viewpoint of ensuring the curability of the adhesive film for forming the first adhesive layer. It may be 10% by mass or more, 15% by mass or more, or 20% by mass or more.
- the content of the component (C) is 70% by mass or less based on the total mass of the first adhesive layer from the viewpoint of ensuring the formability of the adhesive film for forming the first adhesive layer. It may be 60% by mass or less, 50% by mass or less, or 40% by mass or less.
- the content of the component (C) in the composition or the composition layer for forming the first adhesive layer (based on the total mass of the composition or the composition layer) may be the same as the above range.
- the first adhesive layer 2 may further contain other components in addition to the component (A), the cured product of the component (B), and the component (C).
- other components include a thermoplastic resin (hereinafter, may be referred to as “(D) component”), a coupling agent (hereinafter, may be referred to as “(E) component”), and a filler. (Hereinafter, it may be referred to as "(F) component”.) And the like.
- a resin that functions as a film-forming component can be used, and for example, a phenoxy resin, a polyester resin, a polyamide resin, a polyurethane resin, a polyester urethane resin, an acrylic rubber, an epoxy resin (solid at 25 ° C.) and the like can be used. Can be mentioned. These may be used individually by 1 type, and may be used in combination of a plurality of types.
- the composition layer further, the first adhesive layer 2 from the composition. Can be easily formed.
- the component (D) may be, for example, a phenoxy resin.
- the weight average molecular weight (Mw) of the component (D) may be, for example, 5000 to 200,000, 10000 to 100,000, 20000 to 80,000, or 40,000 to 60,000 from the viewpoint of resin exclusion during mounting.
- Mw means a value measured by gel permeation chromatography (GPC) and converted using the calibration curve by standard polystyrene.
- the content of the component (D) may be 1% by mass or more, 5% by mass or more, 10% by mass or more, or 20% by mass or more, 70% by mass, based on the total mass of the first adhesive layer. Hereinafter, it may be 60% by mass or less, 50% by mass or less, or 40% by mass or less.
- the content of the component (D) in the composition or the composition layer for forming the first adhesive layer (based on the total mass of the composition or the composition layer) may be the same as the above range.
- the component (E) examples include a silane coupling agent having an organic functional group such as a (meth) acryloyl group, a mercapto group, an amino group, an imidazole group and an epoxy group, a silane compound such as tetraalkoxysilane, and a tetraalkoxy titanate derivative. , Polydialkyl titanate derivatives and the like. These may be used individually by 1 type, and may be used in combination of a plurality of types. When the first adhesive layer 2 contains the component (E), the adhesiveness can be further improved.
- the component (E) may be, for example, a silane coupling agent.
- the content of the component (E) may be 0.1 to 10% by mass based on the total mass of the first adhesive layer.
- the content of the component (E) in the composition or the composition layer for forming the first adhesive layer (based on the total mass of the composition or the composition layer) may be the same as the above range.
- the component (F) include non-conductive fillers (for example, non-conductive particles).
- the component (F) may be either an inorganic filler or an organic filler.
- the inorganic filler include metal oxide fine particles such as silica fine particles, alumina fine particles, silica-alumina fine particles, titania fine particles, and zirconia fine particles; and inorganic fine particles such as metal nitride fine particles.
- the organic filler include organic fine particles such as silicone fine particles, methacrylate / butadiene / styrene fine particles, acrylic / silicone fine particles, polyamide fine particles, and polyimide fine particles. These may be used individually by 1 type, and may be used in combination of a plurality of types.
- the component (F) can be appropriately blended as long as the effect of the present invention is not impaired, and the content of the component (F) in the composition or composition layer for forming the first adhesive layer. (Based on the total mass of the composition or the composition layer) can also be appropriately set as long as the effect of the present invention is not impaired.
- the first adhesive layer 2 may further contain other additives such as a softener, an accelerator, a deterioration inhibitor, a colorant, a flame retardant, and a thixotropic agent.
- the content of the other additives may be, for example, 0.1 to 10% by mass based on the total mass of the first adhesive layer.
- the content of the composition for forming the first adhesive layer or other additives in the composition layer (based on the total mass of the composition or the composition layer) may be the same as the above range.
- the thickness d1 of the first adhesive layer 2 is 0.1 times or more the average particle size of the conductive particles 4 from the viewpoint that the conductive particles 4 are easily captured between the facing electrodes and the connection resistance can be further reduced. It may be present, 0.2 times or more, and may be 0.3 times or more. The thickness d1 of the first adhesive layer 2 makes it easier for the conductive particles to collapse when the conductive particles are sandwiched between the facing electrodes during thermocompression bonding, and the conductive particles 4 can further reduce the connection resistance.
- the average particle size of the particles may be 0.8 times or less, and may be 0.7 times or less.
- the thickness d1 of the first adhesive layer 2 may be 0.1 to 0.8 times, and 0.2 to 0.8 times, the average particle size of the conductive particles 4. It may be 0.3 to 0.7 times.
- the thickness d1 of the first adhesive layer 2 refers to the thickness of the first adhesive layer located at the separated portion of the adjacent conductive particles 4 and 4.
- the conductive particles in the first adhesive layer 2 A part of 4 may protrude from the first adhesive layer 2 toward the second adhesive layer 3.
- the boundary S between the first adhesive layer 2 and the second adhesive layer 3 is located at the separated portion of the adjacent conductive particles 4 and 4. Due to the presence of the boundary S on the conductive particles along the surface of the conductive particles, the conductive particles 4 in the first adhesive layer 2 are moved from the first adhesive layer 2 to the second adhesive layer 3 side.
- the above relationship may be satisfied without protruding.
- the conductive particles 4 may not be exposed on the surface 2a of the first adhesive layer 2 opposite to the side of the second adhesive layer 3, and the surface 2a on the opposite side may be a flat surface.
- the relationship between the thickness d1 of the first adhesive layer 2 and the maximum particle size of the conductive particles 4 may be the same as described above.
- the thickness d1 of the first adhesive layer 2 may be 0.1 to 0.8 times, 0.2 to 0.8 times, the maximum particle size of the conductive particles 4, and may be 0. It may be 3 to 0.7 times.
- the thickness d1 of the first adhesive layer 2 may be, for example, 5.0 ⁇ m or less.
- the thickness d1 of the first adhesive layer 2 may be 4.5 ⁇ m or less or 4.0 ⁇ m or less.
- the thickness d1 of the first adhesive layer 2 may be, for example, 0.1 ⁇ m or more, 0.5 ⁇ m or more, or 0.7 ⁇ m or more.
- the thickness d1 of the first adhesive layer 2 is determined by, for example, sandwiching an adhesive film between two sheets of glass (thickness: about 1 mm) and bisphenol A type epoxy resin (trade name: JER811, Mitsubishi Chemical Co., Ltd.). After casting with a resin composition consisting of 100 g of diethylenetriamine (manufactured by Tokyo Kasei Kogyo Co., Ltd.) and 10 g of diethylenetriamine, cross-sectional polishing is performed using a polishing machine, and a scanning electron microscope (SEM, trade name: SE-8010,) It can be obtained by measuring using Hitachi High-Tech Science Co., Ltd.). Further, as shown in FIG.
- the first The first adhesive layer 2 and the second adhesive layer 3 located at the separated portions of the adjacent conductive particles 4 and 4 from the surface 2a of the adhesive layer 2 opposite to the second adhesive layer 3 side.
- the distance to the boundary S with and (the distance indicated by d1 in FIG. 1) is the thickness of the first adhesive layer 2, and the exposed portion of the conductive particles 4 is included in the thickness of the first adhesive layer 2. I can't.
- the length of the exposed portion of the conductive particles 4 may be, for example, 0.1 ⁇ m or more, and may be 5.0 ⁇ m or less.
- the second adhesive layer 3 can contain the component (C) and the component (F).
- the component (C1) and the component (C2) used in the component (C) in the second adhesive layer 3 are (C) in the first adhesive layer 2. Since it is the same as the component (C1) and the component (C2) used in the component (that is, the first thermosetting resin component), detailed description thereof will be omitted here.
- the second thermosetting resin component may be the same as or different from the first thermosetting resin component.
- the content of the component (C) is 5% by mass or more, 10% by mass or more, 15% by mass or more, or 20% by mass or more based on the total mass of the second adhesive layer from the viewpoint of maintaining reliability. May be.
- the content of the component (C) is 70% by mass or less and 60% by mass or less based on the total mass of the second adhesive layer from the viewpoint of preventing the resin seepage problem in the reel, which is one aspect of the supply form. , 50% by mass or less, or 40% by mass or less.
- the second adhesive layer 3 can contain an inorganic filler as the component (F). Even when the circuit members are connected to each other at low pressure, sufficient continuity can be ensured between the facing electrodes of the circuit connection structure, and large indentations that cause defect determination of the automatic visual inspection device are sufficiently generated. From the viewpoint of suppression, the second adhesive layer 3 has a particle size D50 at 50% cumulative size of 0.5 to 1.0 ⁇ m in a volume-based particle size distribution, and a particle size D95 at 95% cumulative size is 0. It can be formed from a thermosetting composition containing an inorganic filler having a size of 9 to 2.0 ⁇ m.
- a silica filler such as silica fine particles can be used from the viewpoint of improving reliability.
- the content of silica in the silica filler may be 99% by mass or more, or 100% by mass, based on the total amount of the silica filler.
- the inorganic filler having the above-mentioned volume-based particle size distribution is, for example, an inorganic filler containing inorganic particles having a primary particle size of 0.3 to 0.7 ⁇ m, or an inorganic filler having a volume average particle size of 1.0 to 2.0 ⁇ m.
- the D50 of the inorganic filler may be 0.5 to 1.0 ⁇ m, 0.6 to 0.9 ⁇ m, or 0.7 to 0.8 ⁇ m. There may be. Further, from the viewpoint of suppressing the generation of large indentations, the D95 of the inorganic filler may be 0.9 to 2.0 ⁇ m, 1.0 to 1.8 ⁇ m, or 1.1 to 1. It may be 6 ⁇ m.
- the content of the filler may be 10 to 70% by mass, 20 to 60% by mass, or 30 to 50% based on the total mass of the second adhesive layer or the thermosetting composition. It may be% by mass.
- the second adhesive layer 3 may further contain other components and other additives in the first adhesive layer 2. Preferred embodiments of the other components and other additives are the same as the preferred embodiments of the first adhesive layer 2.
- the content of the component (D) may be 1% by mass or more, 5% by mass or more, or 10% by mass or more, and is 80% by mass or less and 60% by mass, based on the total mass of the second adhesive layer. It may be less than or equal to 40% by mass or less.
- the content of the component (E) may be 0.1 to 10% by mass based on the total mass of the second adhesive layer.
- the content of the other additives may be, for example, 0.1 to 10% by mass based on the total mass of the second adhesive layer.
- the thickness d2 of the second adhesive layer 3 may be appropriately set according to the height of the electrodes of the circuit member to be adhered.
- the thickness d2 of the second adhesive layer 3 is 5 ⁇ m or more or 7 ⁇ m or more from the viewpoint that the space between the electrodes can be sufficiently filled to seal the electrodes and better connection reliability can be obtained. It may be 15 ⁇ m or less or 11 ⁇ m or less.
- the thickness d2 of the second adhesive layer 3 can be obtained, for example, by the same method as the method for measuring the thickness d1 of the first adhesive layer 2.
- the first in the second adhesive layer 3 The distance from the surface 3a on the side opposite to the adhesive layer 2 side to the boundary S between the first adhesive layer 2 and the second adhesive layer 3 located at the separated portions of the adjacent conductive particles 4 and 4 ( The distance (d2) in FIG. 1 is the thickness of the second adhesive layer 3.
- the third adhesive layer 6 can contain the component (C).
- the component (C1) and the component (C2) used in the component (C) in the third adhesive layer (that is, the third thermosetting resin component) are the component (C) in the first adhesive layer 2. Since it is the same as the component (C1) and the component (C2) used in (that is, the first thermosetting resin component), detailed description thereof will be omitted here.
- the third thermosetting resin component may be the same as or different from the first thermosetting resin component.
- the third thermosetting resin component may be the same as or different from the second thermosetting resin component.
- the content of the component (C) is 5% by mass or more, 10% by mass or more, and 15% by mass or more based on the total mass of the third adhesive layer from the viewpoint of imparting good transferability and peeling resistance. , Or 20% by mass or more.
- the content of the component (C) is 70% by mass or less based on the total mass of the third adhesive layer from the viewpoint of imparting good half-cut property and blocking resistance (suppression of resin seepage of the reel). It may be 60% by mass or less, 50% by mass or less, or 40% by mass or less.
- the third adhesive layer may further contain other components and other additives in the first adhesive layer 2.
- the content of the component (D) may be 10% by mass or more, 20% by mass or more, or 30% by mass or more, and is 80% by mass or less and 70% by mass, based on the total mass of the third adhesive layer. It may be less than or equal to 60% by mass or less.
- the content of the component (E) may be 0.1 to 10% by mass based on the total mass of the third adhesive layer.
- the content of the component (F) can be appropriately set as long as the effect of the present invention is not impaired.
- the content of the other additives may be, for example, 0.1 to 10% by mass based on the total mass of the third adhesive layer.
- the thickness of the third adhesive layer may be appropriately set according to the minimum melt viscosity of the adhesive film, the height of the electrodes of the circuit members to be adhered, and the like.
- the thickness of the third adhesive layer is preferably smaller than the thickness d2 of the second adhesive layer 3.
- the thickness of the third adhesive layer may be 0.2 ⁇ m or more from the viewpoint that the space between the electrodes can be sufficiently filled to seal the electrodes and better connection reliability can be obtained. , 3.0 ⁇ m or less.
- the thickness of the third adhesive layer can be obtained, for example, by the same method as the method for measuring the thickness d1 of the first adhesive layer 2.
- the thicknesses of the adhesive films 1a and 1b (the total thickness of all the layers constituting the adhesive films 1a and 1b, in FIG. 1A, the thicknesses d1 and the first of the first adhesive layers 2). 2 is the total thickness d2 of the adhesive layer 3, and in FIG. 1B, the total thickness of the third adhesive layer) may be, for example, 5 ⁇ m or more or 8 ⁇ m or more. , 30 ⁇ m or less or 20 ⁇ m or less.
- the first adhesive layer may be the above-mentioned region P.
- the range of the region P in the thickness direction of the film can be the same as the thickness d1 of the first adhesive layer 2 described above.
- the region P can be formed by a composition obtained by removing conductive particles from the composition for forming the first adhesive layer described above.
- the second adhesive layer may be the above-mentioned region A.
- the range of the region A in the thickness direction of the film can be the same as the thickness d2 of the second adhesive layer 3 described above.
- the region A can be formed by the composition for forming the second adhesive layer described above.
- the second adhesive layer, or the second adhesive layer and the third adhesive layer may be a region S that does not contain conductive particles.
- the region S can be formed by the composition for forming the second adhesive layer and the composition for forming the third adhesive layer described above.
- the particle size D50 at 50% cumulative size is 0.5 to 1.0 ⁇ m and the particle size D95 at 95% cumulative size is 0.9 to 2.0 ⁇ m in the volume-based particle size distribution.
- the inorganic filler is contained in the second adhesive layer, and may not be contained in the first adhesive layer and the third adhesive layer.
- the minimum melt viscosity of the adhesive films 1a and 1b is 450 to 1600 Pa ⁇ s.
- the minimum melt viscosity of the adhesive films 1a and 1b may be 500 Pa ⁇ s or more, 600 Pa ⁇ s or more, 700 Pa ⁇ s or more, or 800 Pa ⁇ s or more.
- the minimum melt viscosity of the adhesive films 1a and 1b is 450 Pa ⁇ s or more, it is possible to suppress the deformation of the plastic substrate during thermocompression bonding and prevent the occurrence of circuit disconnection.
- the minimum melt viscosity of the adhesive films 1a and 1b may be 1500 Pa ⁇ s or less, 1400 Pa ⁇ s or less, 1300 Pa ⁇ s or less, 1200 Pa ⁇ s or less, 1100 Pa ⁇ s or less, or 1000 Pa ⁇ s or less.
- the minimum melt viscosity of the adhesive films 1a and 1b is 1600 Pa ⁇ s or less, it is possible to suppress the deterioration of the resin exclusion property at the time of circuit connection, so that the connection resistance between the facing electrodes of the circuit connection structure is reduced. It is possible to ensure good conduction characteristics.
- the minimum melt viscosity of the adhesive film can be obtained, for example, by the following method.
- Each adhesive film is laminated with a laminator so as to have a thickness of 200 ⁇ m or more to obtain a laminated body.
- the release-treated PET is peeled off from the obtained laminate and cut into 10.0 mm ⁇ 10.0 mm to obtain a measurement sample.
- the minimum melt viscosity of the obtained measurement sample is measured using a viscoelasticity measuring device (trade name: ARES-G2, manufactured by TA Instruments, Inc., heating rate: 10 ° C./min).
- the second adhesive layer 3 is usually thicker than the first adhesive layer 2. Therefore, the minimum melt viscosity of the adhesive films 1a and 1b tends to fluctuate depending on the second adhesive layer 3.
- the minimum melt viscosity of the adhesive films 1a and 1b can be adjusted, for example, by adjusting the type and content of the constituent components (particularly, the component (D)) contained in the second adhesive layer 3. Further, the minimum melt viscosity of the adhesive films 1a and 1b can also be adjusted, for example, by blending the above-mentioned inorganic filler A as the component (F). By blending the inorganic filler A in the second adhesive layer 3, the minimum melt viscosity can be reduced while sufficiently suppressing the generation of large indentations.
- the adhesive films 1a and 1b are anisotropically conductive adhesive films having anisotropic conductivity.
- the adhesive films 1a and 1b are interposed between the first circuit member having the first electrode and the second circuit member having the second electrode, and the first circuit member and the second circuit member are interposed. Is thermally crimped and used to electrically connect the first electrode and the second electrode to each other.
- the adhesive films 1a and 1b by setting the second adhesive layer 3 as the region A, even when the circuit members are connected to each other at low pressure, between the facing electrodes of the circuit connection structure. Continuity can be ensured, and the generation of large indentations that cause defect determination by the automatic visual inspection device can be sufficiently suppressed.
- the circuit connection adhesive film of this embodiment can be suitably used for COP mounting. More specifically, it can be suitably used for connecting a plastic substrate on which a circuit electrode (for example, an electrode containing Ti) is formed in an organic EL display to an IC chip such as a drive IC.
- a circuit electrode for example, an electrode containing Ti
- the method for producing an adhesive film for circuit connection is, for example, a component (A), a component (B), and a component (C) (first thermosetting resin component), and if necessary, other components.
- the component (C) (third thermosetting resin component), and if necessary, the inorganic filler A and others are placed on the opposite side of the first adhesive layer from the second adhesive layer.
- a step of laminating a third adhesive layer containing the above components (third step) may be further provided.
- the second step may be performed first, or the third step may be performed first.
- the third adhesive layer is laminated on the side opposite to the side where the second adhesive layer of the first adhesive layer is to be laminated.
- FIG. 2 is a schematic cross-sectional view showing a manufacturing method including the above steps.
- a composition containing the component (A), the component (B), and the component (C), and an additive added as needed is stirred and mixed in an organic solvent.
- a varnish composition (a varnish-like first adhesive composition) is prepared by dissolving or dispersing by kneading or the like. Then, the varnish composition is applied onto the mold-released substrate using a knife coater, roll coater, applicator, comma coater, die coater, etc., and then the organic solvent is volatilized by heating to form the substrate. Form a composition layer composed of the composition. At this time, the thickness of the finally obtained first adhesive layer (first adhesive film) can be adjusted by adjusting the coating amount of the varnish composition.
- the composition layer made of the composition is irradiated with light to cure the component (B) in the composition layer, and a first adhesive layer is formed on the substrate.
- the first adhesive layer can be said to be the first adhesive film.
- the organic solvent used in the preparation of the varnish composition is not particularly limited as long as it has the property of uniformly dissolving or dispersing each component.
- examples of such an organic solvent include toluene, acetone, methyl ethyl ketone, methyl isobutyl ketone, ethyl acetate, propyl acetate, butyl acetate and the like. These organic solvents can be used alone or in combination of two or more.
- Stirring and mixing or kneading in the preparation of the varnish composition can be carried out by using, for example, a stirrer, a raider, a three-roll, a ball mill, a bead mill, a homodisper or the like.
- the base material is not particularly limited as long as it has heat resistance that can withstand the heating conditions when volatilizing the organic solvent.
- a substrate examples include stretched polypropylene (OPP), polyethylene terephthalate (PET), polyethylene naphthalate, polyethylene isophthalate, polyvinylidene terephthalate, polyolefin, polyacetate, polycarbonate, polyphenylene sulfide, polyamide, polyimide, cellulose, and the like.
- a substrate (for example, a film) made of an ethylene / vinyl acetate copolymer, polyvinyl chloride, polyvinylidene chloride, a synthetic rubber system, a liquid crystal polymer or the like can be used.
- the heating conditions for volatilizing the organic solvent from the varnish composition applied to the base material can be appropriately set according to the organic solvent to be used and the like.
- the heating conditions may be, for example, 40 to 120 ° C. for 0.1 to 10 minutes.
- a part of the solvent may remain in the first adhesive layer without being removed.
- the content of the solvent in the first adhesive layer may be, for example, 10% by mass or less based on the total mass of the first adhesive layer.
- the content of the component (B) in the varnish composition may be 10% by mass or more and less than 60% by mass based on the total of the components (A) and the components other than the organic solvent of the varnish composition.
- the effect of suppressing the flow of the conductive particles can be easily obtained, and the coating can be easily performed while maintaining a good appearance.
- irradiation light for example, ultraviolet light
- Light irradiation can be performed using, for example, a low-pressure mercury lamp, a medium-pressure mercury lamp, a high-pressure mercury lamp, an ultra-high-pressure mercury lamp, a xenon lamp, a metal halide lamp, an LED light source, or the like.
- the integrated light amount of light irradiation can be appropriately set, but may be, for example, 500 to 3000 mJ / cm 2 .
- the second step is a step of laminating the second adhesive layer on the first adhesive layer.
- the second adhesive is applied onto the substrate in the same manner as in the first step, except that the component (C) and the inorganic filler A are used and no light irradiation is performed.
- a layer is formed to obtain a second adhesive film.
- the second adhesive layer 3 provided on the base material 20 as shown in FIG. 2A can be prepared.
- the second adhesive layer can be laminated on the first adhesive layer by adhering the first adhesive film and the second adhesive film (FIGS. 2A and 2). b)).
- a varnish composition obtained by using the component (C), the inorganic filler A, and other additives added as needed on the first adhesive layer.
- the second adhesive layer can also be laminated on the first adhesive layer by applying the second adhesive composition in the form) and volatilizing the organic solvent.
- Examples of the method of adhering the first adhesive film and the second adhesive film include a method of heat pressing, roll laminating, vacuum laminating and the like. Lamination can be performed, for example, under temperature conditions of 0 to 80 ° C.
- a part of the solvent may remain on the second adhesive layer without being removed.
- the content of the solvent in the second adhesive layer may be, for example, 10% by mass or less based on the total mass of the second adhesive layer.
- the third step is a step of laminating the third adhesive layer on the side of the first adhesive layer opposite to the second adhesive layer.
- a third adhesive layer is formed on the substrate to obtain a third adhesive film.
- the third adhesive layer 6 provided on the base material 24 as shown in FIG. 2 (c) can be prepared.
- the side of the first adhesive layer opposite to the second adhesive layer A third adhesive layer can be laminated on top (see (c) in FIG. 2).
- the varnish composition (the varnish-like third adhesion) is placed on the opposite side of the first adhesive layer from the second adhesive layer.
- the third adhesive layer can also be laminated on the first adhesive layer by applying the agent composition) and volatilizing the organic solvent. The method of bonding and the conditions thereof are the same as in the second step.
- a part of the solvent may remain on the third adhesive layer without being removed.
- the content of the solvent in the third adhesive layer may be, for example, 10% by mass or less based on the total mass of the third adhesive layer.
- composition containing inorganic filler In the composition containing an inorganic filler of the present embodiment, the particle size D50 at 50% cumulative size is 0.5 to 1.0 ⁇ m and the particle size D95 at 95% cumulative size is 0.9 to 2 in the volume-based particle size distribution. Contains an inorganic filler that is 0.0 ⁇ m. As the inorganic filler, the same as the above-mentioned inorganic filler A can be used.
- the inorganic filler-containing composition of the present embodiment can be used to form an inorganic filler-containing region in a circuit connection member containing conductive particles and an inorganic filler.
- the circuit connection member include the above-mentioned circuit connection adhesive film.
- the above-mentioned region A and the second adhesive layer can be formed as the inorganic filler-containing region.
- composition of the inorganic filler-containing composition of the present embodiment can be set in the same manner as the composition of the second adhesive layer described above.
- the composition may further contain a thermoplastic resin.
- the inorganic filler-containing composition of the present embodiment may be a varnish composition containing the above-mentioned organic solvent (varnish-like inorganic filler-containing composition).
- the inorganic filler-containing composition of the present embodiment can be used to form an adhesive layer having a thickness of 10 ⁇ m or less, 9 to 4 ⁇ m, or 8 to 5 ⁇ m. According to the composition containing an inorganic filler of the present embodiment, even when coating with such a design thickness, appearance defects such as scratches are unlikely to occur, and a high coating yield can be obtained.
- FIG. 3 is a schematic cross-sectional view showing an embodiment of a circuit connection structure.
- the circuit connection structure 10 includes a first circuit member 13 having a first electrode 12 formed on a main surface 11a of the first circuit board 11 and the first circuit board 11.
- a second circuit member 16 having a second electrode 15 formed on the main surface 14a of the second circuit board 14 and the second circuit board 14, and the first circuit member 13 and the second circuit member. It is arranged between 16 and includes a circuit connection portion 17 that electrically connects the first electrode 12 and the second electrode 15 to each other.
- the first circuit member 13 and the second circuit member 16 may be the same or different from each other.
- the first circuit member 13 and the second circuit member 16 are a glass substrate or a plastic substrate on which a circuit electrode is formed; a printed wiring board; a ceramic wiring board; a flexible wiring board; an IC chip such as a drive IC, or the like. It's okay.
- the first circuit board 11 and the second circuit board 14 may be formed of an inorganic substance such as semiconductor, glass, or ceramic, an organic substance such as polyimide or polycarbonate, or a composite such as glass / epoxy.
- the first circuit board 11 may be a plastic substrate.
- the first circuit member 13 may be, for example, a plastic substrate on which a circuit electrode is formed (a plastic substrate made of an organic substance such as polyimide, polycarbonate, polyethylene terephthalate, or cycloolefin polymer), and the second circuit member 16 may be.
- a plastic substrate on which a circuit electrode is formed a plastic substrate made of an organic substance such as polyimide, polycarbonate, polyethylene terephthalate, or cycloolefin polymer
- the second circuit member 16 may be.
- it may be an IC chip such as a drive IC.
- a display region is formed by regularly arranging a pixel drive circuit such as an organic TFT or a plurality of organic EL elements R, G, and B on the plastic substrate in a matrix. It may be a plastic one.
- the first electrode 12 and the second electrode 15 are gold, silver, tin, ruthenium, rhodium, palladium, osmium, iridium, platinum, copper, aluminum, molybdenum, titanium and other metals, indium tin oxide (ITO), and the like.
- the electrode may be an electrode containing an oxide such as indium tin oxide (IZO) or indium gallium zinc oxide (IGZO).
- the first electrode 12 and the second electrode 15 may be electrodes formed by laminating two or more of these metals, oxides, and the like.
- the electrode formed by stacking two or more types may have two or more layers, and may have three or more layers.
- the first electrode 12 When the first circuit member 13 is a plastic substrate, the first electrode 12 may be an electrode containing Ti, and more specifically, an electrode having a titanium layer on the outermost surface.
- the first electrode 12 and the second electrode 15 may be circuit electrodes or bump electrodes. At least one of the first electrode 12 and the second electrode 15 may be a bump electrode. In FIG. 3, the first electrode 12 is a circuit electrode and the second electrode 15 is a bump electrode.
- the circuit connection portion 17 contains the cured product of the adhesive film 1a described above.
- the circuit connection portion 17 may be made of the cured product of the adhesive film 1a described above.
- the circuit connection portion 17 is located, for example, on the side of the first circuit member 13 in the direction in which the first circuit member 13 and the second circuit member 16 face each other (hereinafter referred to as “opposite direction”), and the above-mentioned first circuit member 17 is located. It is located on the side of the first region 18 composed of the cured product of the component (B) and the cured product of the component (C) other than the conductive particles 4 in the adhesive layer of No. 1 and the second circuit member 16 in the opposite direction.
- the first electrode 12 and the first electrode 12 are interposed between the second region 19 made of a cured product such as the component (C) in the second adhesive layer and at least the first electrode 12 and the second electrode 15. It has conductive particles 4 that electrically connect the second electrodes 15 to each other. As shown in FIG. 3, the circuit connection portion 17 does not have to have two distinct regions between the first region 18 and the second region 19, and the first adhesive layer The cured product derived from the above and the cured product derived from the second adhesive layer may be mixed to form one region.
- the circuit connection structure may be a plastic substrate in which one of the first circuit member and the second circuit member is an IC chip and the other has an electrode containing Ti.
- the circuit connection structure is, for example, a flexible organic electric field light emitting color display (organic EL display) in which a plastic substrate in which organic EL elements are regularly arranged and a drive circuit element which is a driver for displaying an image are connected. Examples thereof include a touch panel in which a plastic substrate on which organic EL elements are regularly arranged and a position input element such as a touch pad are connected.
- the circuit connection structure can be applied to various monitors such as smart phones, tablets, televisions, vehicle navigation systems, wearable terminals, furniture; home appliances; daily necessities and the like.
- FIG. 4 is a schematic cross-sectional view showing an embodiment of a method for manufacturing a circuit connection structure.
- FIG. 4A and FIG. 4B are schematic cross-sectional views showing each step.
- a method of manufacturing the circuit connection structure 10 is performed between a first circuit member 13 having a first electrode 12 and a second circuit member 16 having a second electrode 15.
- a first electrode 12 having a first electrode 12 formed on a main surface 11a of the first circuit board 11 and the first circuit board 11 is provided.
- a circuit member 13 and a second circuit member 16 provided with a second electrode 15 formed on the main surface 14a of the second circuit board 14 and the second circuit board 14 are prepared.
- the first circuit member 13 and the second circuit member 16 are arranged so that the first electrode 12 and the second electrode 15 face each other, and the first circuit member 13 and the second circuit member 12 are arranged.
- the adhesive film 1a is placed between the 16 and 16.
- the adhesive film 1a is placed on the first circuit member 13 so that the first adhesive layer 2 side faces the main surface 11a of the first circuit board 11. Laminate.
- the adhesive film 1a is laminated so that the first electrode 12 on the first circuit board 11 and the second electrode 15 on the second circuit board 14 face each other.
- the second circuit member 16 is arranged on the circuit member 13.
- the first circuit member 13 and the second circuit member 16 are heated while heating the first circuit member 13, the adhesive film 1a, and the second circuit member 16.
- the first circuit member 13 and the second circuit member 16 are thermocompression bonded to each other.
- the second adhesive layer 3 has a flowable uncured thermosetting component
- the second electrodes 15 are connected to each other. It flows so as to fill the voids of the above, and is cured by the above heating.
- the first electrode 12 and the second electrode 15 are electrically connected to each other via the conductive particles 4, and the first circuit member 13 and the second circuit member 16 are adhered to each other.
- the circuit connection structure 10 shown in 3 can be obtained.
- a part of the first adhesive layer 2 is cured by light irradiation, so that the conductive particles in the first adhesive layer 2 flow. It is suppressed, the first adhesive layer 2 hardly flows during the thermal pressure bonding, and the conductive particles are efficiently captured between the facing electrodes. Therefore, between the facing first electrodes 12 and the second electrodes 15. Connection resistance is reduced. Further, when the thickness of the first adhesive layer is 5 ⁇ m or less, the conductive particles at the time of circuit connection tend to be captured more efficiently.
- the heating temperature for thermocompression bonding can be set as appropriate, but may be, for example, 50 to 190 ° C.
- the pressurization is not particularly limited as long as it does not damage the adherend, but in the case of COP mounting, for example, the area conversion pressure at the bump electrode may be 0.1 to 50 MPa, and may be 40 MPa or less. It may be 0.1 to 40 MPa. Further, in the case of COG mounting, for example, the area conversion pressure at the bump electrode may be 10 to 100 MPa.
- (B) component Photocurable resin component (B1) component: Radical polymerizable compound B1-1: NK ester A-BPEF70T (ethoxylated fluorene type di (meth) acrylate (bifunctional), manufactured by Shin-Nakamura Chemical Industry Co., Ltd.) ), Diluted with toluene to 70% by mass of non-volatile content B1-2: Lipoxy VR-90 (bisphenol A type epoxy (meth) acrylate (bifunctional) (vinyl ester resin), manufactured by Showa Denko Co., Ltd.)
- Photoradical Polymerization Initiator B2-1 Acetyl OXE-02 (Etanon, 1- [9-ethyl-6- (2-methylbenzoyl) -9H-carbazole-3-yl]-, 1-( 0-Acetyl oxime), manufactured by BASF), MEK diluted to 10% by mass of non-volatile content
- C component Thermosetting resin component (C1) component: Cationic polymerizable compound
- C1-1 ETERNACOLL OXBP (3-ethyl-3-hydroxymethyloxetane, manufactured by Ube Industries, Ltd.)
- C1-2 EHPE3150 (1,2-epoxy-4- (2-oxylanyl) cyclohexane adduct of 2,2-bis (hydroxymethyl) -1-butanol, manufactured by Daicel Corporation)
- C1-3 Celoxide 2021P (3,4-epoxycyclohexylmethyl (3,4-epoxy) cyclohexanecarboxylate, manufactured by Daicel Corporation)
- C1-4 OXSQ-TX100 (poly ( ⁇ 3-[(3-ethyl-3-oxetanyl) methoxy] propyl ⁇ silsesquioxane) derivative, manufactured by Toagosei Corporation)
- C1-5 Celoxide 8010 (B-7-oxavicyclo
- Epoxy resin D-1 Phenototo YP-50S (bisphenol A type phenoxy resin, weight average molecular weight: 60,000, glass transition temperature: 84 ° C., manufactured by Nittetsu Chemical & Materials Co., Ltd.), MEK D-2: TOPR-300 (high Tg type epoxy resin, epoxy equivalent: 900-1,000, softening point: 120 ° C, manufactured by Nittetsu Chemical & Materials Co., Ltd.) D-3: Phenototo FX-293 (fluorene skeleton-containing phenoxy resin, weight average molecular weight: 45,000, glass transition temperature: 158 ° C, Nittetsu Chemical & Materials Made by MEK, diluted to 60% by mass of non-volatile content D-4: Phenototo ZX-1356-2 (bisphenol A type and bisphenol F type copolymer phenoxy resin, weight average molecular weight: 70000, Glass transition temperature: 71 ° C, manufactured
- F Component: Filler (F1)
- F-3 Admanano YA050C (silica filler, stock) (Manufactured by Admatex), use MEK diluted to 50% by mass of non-volatile content
- the particle size D50 at the time of 50% accumulation (particle size of the cumulative distribution 50% by volume) and the particle size D95 at the time of 95% accumulation (particle size of the cumulative distribution 95% by volume) were measured. ..
- Microtorac MT3300EXII manufactured by Nikkiso Co., Ltd. was used as a measuring device, and methyl ethyl ketone was used as a measuring solvent.
- a PET (polyethylene terephthalate) film obtained by mixing the materials shown in Table 2 with the composition ratio (mass ratio) shown in Table 2 (the numerical values in Table 2 mean the non-volatile content) and then performing a mold release treatment.
- a composition layer composed of a composition containing each component was obtained by applying the coating on the above while applying a magnetic field and drying the organic solvent or the like at 70 ° C. for 5 minutes with hot air. The composition layer was coated so that the thickness after drying was 3 to 4 ⁇ m, respectively.
- a first adhesive layer in which conductive particles were dispersed was prepared.
- the thickness was measured using a contact thickness gauge.
- the thickness of the layer made of the first adhesive composition or the adhesive layer is smaller than the thickness (diameter) of the conductive particles
- the thickness of the layer is measured using a contact type thickness gauge, and the conductive particles are measured.
- the thickness of the region where the conductive particles are present is measured. Therefore, after producing a two-layer adhesive film in which a first adhesive layer and a second adhesive layer are laminated, an adhesive particle having adjacent conductive particles is used by a scanning electron microscope by a method described later. The thickness of the first adhesive layer located at the separated portion was measured.
- a second adhesive layer composed of a composition containing each component was prepared by coating on the above and drying an organic solvent or the like at 70 ° C. for 5 minutes with hot air. The adhesive layer was coated so that the thickness after drying was 8 to 9 ⁇ m, respectively. The thickness here was measured using a contact thickness gauge.
- the ratio Y (%) at which white lines and scratches did not occur was determined and evaluated according to the following criteria.
- a third adhesive layer made of a composition containing each component was prepared by coating on the above and drying an organic solvent or the like at 70 ° C. for 5 minutes with hot air. The adhesive layer was coated so that the thickness after drying was 0.5 to 1.5 ⁇ m, respectively. The thickness here was measured using a contact thickness gauge.
- Example 1 (Examples 1 to 5 and Comparative Examples 1 to 5) [Preparation of adhesive film]
- an adhesive film having the constitution shown in Table 6 was prepared.
- the first adhesive layer formed by the composition P-1 is heated to a temperature of 50 to 60 ° C. on the second adhesive layer formed by the composition S1-1.
- the PET film on the first adhesive layer side was peeled off.
- the third adhesive layer formed by the composition S2-1 was bonded to the exposed first adhesive layer while applying a temperature of 50 to 60 ° C. to obtain the adhesive film of Example 1. ..
- the peeling force between the second adhesive layer and the PET film is the first adhesion.
- Each PET film was selected so as to be larger than the peeling force between the agent layer and the PET film and the peeling force between the third adhesive layer and the PET film.
- Example 2 to 4 and Comparative Examples 1 to 4 the adhesive films having the configurations shown in Table 6 were prepared in the same manner as in Example 1.
- Example 5 and Comparative Example 5 an adhesive film having the constitution shown in Table 6 was prepared in the same manner as in Example 1 except that the third adhesive layer was not bonded.
- the thickness of the first adhesive layer of the produced adhesive film for circuit connection was measured by the following method. First, an adhesive film for circuit connection is sandwiched between two sheets of glass (thickness: about 1 mm), and 100 g of bisphenol A type epoxy resin (trade name: JER811, manufactured by Mitsubishi Chemical Industry Co., Ltd.) and diethylenetriamine (manufactured by Tokyo Chemical Industry Co., Ltd.). ) was cast with a resin composition consisting of 10 g. After that, the cross section is polished using a polishing machine, and a scanning electron microscope (SEM, trade name: SE-8010, manufactured by Hitachi High-Tech Science Co., Ltd.) is used to perform the first section located at the separated portion of the adjacent conductive particles. The thickness of the adhesive layer was measured. The thickness of the first adhesive layer was 1.8 ⁇ m.
- circuit connection structure-1 As the first circuit member, an IC chip (0.9 mm ⁇ 20.3 mm, thickness: 0.3 mm, bump electrode size: 70 ⁇ m ⁇ 12 ⁇ m, space between bump electrodes) in which bump electrodes are arranged in two rows in a staggered pattern. : 12 ⁇ m, bump electrode thickness: 9 ⁇ m) was prepared. Further, as a second circuit member, a wiring pattern (pattern width) of Ti: 50 nm / Al: 400 nm is provided on the surface of a polyimide substrate (manufactured by Toray DuPont Co., Ltd., 200H) (38 mm ⁇ 28 mm, thickness: 0.05 mm). : 19 ⁇ m, space between electrodes: 5 ⁇ m) was prepared.
- a polyimide substrate manufactured by Toray DuPont Co., Ltd., 200H
- Circuit connection structures were produced using the adhesive films of Examples 1 to 5 and Comparative Examples 1 to 5.
- the adhesive film is cut into a width of 2.0 mm, and the adhesive film is in contact with the third adhesive layer (second adhesive layer in the case of Example 5 and Comparative Example 5) and the first circuit member.
- a thermocompression bonding device consisting of a stage consisting of a ceramic heater and a tool (8 mm ⁇ 50 mm
- heating and pressurization were performed for 2 seconds at 70 ° C. and 0.98 MPa (10 kgf / cm 2 ), and the first step was performed.
- An adhesive film was attached to the circuit member, and the release film on the side opposite to the first circuit member of the adhesive film was peeled off.
- a heat tool was used at 8 mm ⁇ 45 mm, and Teflon (registered trademark) having a thickness of 50 ⁇ m was used as a cushioning material.
- Teflon registered trademark
- the first adhesive layer of the adhesive film is attached to the second circuit member by heating and pressurizing the adhesive film for 5 seconds under the conditions of the actual measured maximum reached temperature of 170 ° C. and the area conversion pressure of 30 MPa at the bump electrode. Then, the circuit connection structure-1 was manufactured.
- an IC chip (0.9 mm ⁇ 20.3 mm, thickness: 0.3 mm, bump electrode size: 70 ⁇ m ⁇ 12 ⁇ m, space between bump electrodes) in which bump electrodes are arranged in two rows in a staggered pattern. : 12 ⁇ m, bump electrode thickness: 5 ⁇ m) was prepared.
- a glass substrate (25 mm ⁇ 35 mm, thickness: 0.2 mm) having an Al / Nd film having a thickness of 150 nm was prepared on the surface of the glass substrate (25 mm ⁇ 35 mm, thickness: 0.2 mm).
- the adhesive films of Examples 1 to 5 and Comparative Examples 1 to 5 were used in the same manner as in the production of the circuit connection structure-1 except that the first circuit member and the second circuit member were used.
- the circuit connection structure-2 was manufactured.
- connection resistance (conduction resistance) of the produced circuit connection structure-1 was measured by the 4-terminal method. A multimeter MLR21 manufactured by Kusumoto Kasei Co., Ltd. was used for the measurement. The potential difference was measured at any 14 points, and the average value was obtained. The average value of the potential difference was converted into the connection resistance value and evaluated according to the following criteria. The results are shown in Table 6.
- C Connection resistance value is 1.0 ⁇ or more
- a PET (polyethylene terephthalate) film obtained by mixing the materials shown in Table 7 with the composition ratio (mass ratio) shown in Table 7 (the numerical values in Table 7 mean the non-volatile content) and then performing a mold release treatment.
- a composition layer composed of a composition containing each component was obtained by coating on the above and drying an organic solvent or the like at 70 ° C. for 5 minutes with hot air. The composition layer was coated so as to have a thickness of 5 ⁇ m after drying to prepare a first adhesive layer-B. The thickness here was measured using a contact thickness gauge.
- a second adhesive layer-B made of a composition containing each component was prepared by coating on the above and drying an organic solvent or the like at 70 ° C. for 5 minutes with hot air. The adhesive layer was coated so that the thickness after drying was 11 ⁇ m each. The thickness here was measured using a contact thickness gauge.
- the ratio Y (%) at which white lines and scratches did not occur was determined and evaluated according to the following criteria.
- Example 6 and Comparative Examples 6 to 8 [Preparation of adhesive film] Using the first adhesive layer-B and the second adhesive layer-B prepared above, an adhesive film having the constitution shown in Table 9 was prepared.
- the adhesive film of Example 6 50 to 60 first adhesive layers-B formed by the composition P-2 are added to the second adhesive layer-B formed by the composition S1-9.
- the adhesive film of Example 6 was obtained by laminating while applying a temperature of ° C.
- an IC chip (0.9 mm ⁇ 20.3 mm, thickness: 0.3 mm, bump electrode size: 70 ⁇ m ⁇ 12 ⁇ m, space between bump electrodes) in which bump electrodes are arranged in two rows in a staggered pattern. : 12 ⁇ m, bump electrode thickness: 5 ⁇ m) was prepared.
- a glass substrate (25 mm ⁇ 35 mm, thickness: 0.2 mm) having a Ti / Al / Ti film having a thickness of 150 nm was prepared on the surface of the glass substrate (25 mm ⁇ 35 mm, thickness: 0.2 mm).
- a circuit connection structure was produced using each of the adhesive films of Examples 6 and Comparative Examples 6 to 8.
- the adhesive film was cut out to a width of 2.0 mm, and the adhesive film was placed on the first circuit member so that the second adhesive layer-B and the first circuit member were in contact with each other.
- a thermocompression bonding device consisting of a stage consisting of a ceramic heater and a tool (8 mm ⁇ 50 mm)
- heating and pressurization were performed for 2 seconds at 70 ° C. and 0.98 MPa (10 kgf / cm 2 ), and the first step was performed.
- An adhesive film was attached to the circuit member, and the release film on the side opposite to the first circuit member of the adhesive film was peeled off.
- a heat tool was used at 8 mm ⁇ 45 mm, and Teflon (registered trademark) having a thickness of 50 ⁇ m was used as a cushioning material.
- Teflon registered trademark
- the first adhesive layer of the adhesive film is attached to the second circuit member by heating and pressurizing for 5 seconds under the conditions of the measured maximum reached temperature of the adhesive film of 145 ° C. and the area conversion pressure of 30 MPa at the bump electrode. Then, the circuit connection structure-3 was manufactured.
- connection resistance (Evaluation of connection resistance) The initial connection resistance (conduction resistance) of the produced circuit connection structure-3 was measured by the 4-terminal method. A multimeter MLR21 manufactured by Kusumoto Kasei Co., Ltd. was used for the measurement. The potential difference was measured at any 14 points, and the average value was obtained. The average value of the potential difference was converted into the connection resistance value and evaluated according to the following criteria. The results are shown in Table 9. A: Connection resistance value is less than 5 ⁇ B: Connection resistance value is 5 ⁇ or more and less than 10 ⁇ C: Connection resistance value is 10 ⁇ or more
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Abstract
Description
本実施形態の回路接続用接着剤フィルムは、導電粒子を含み、フィルムの厚さ方向において、無機フィラーを含有する領域Aを含み、領域Aは、体積基準の粒度分布における50%累積時の粒径D50が0.5~1.0μmであり、95%累積時の粒径D95が0.9~2.0μmである無機フィラー(以下、「無機フィラーA」という場合がある。)を含有する熱硬化性組成物から形成されている。領域Aを形成する熱硬化性組成物は、重合性化合物と、熱重合開始剤とを含むことができる。 <Adhesive film for circuit connection>
The circuit connection adhesive film of the present embodiment contains conductive particles and contains a region A containing an inorganic filler in the thickness direction of the film, and the region A is a particle at 50% accumulation in the volume-based particle size distribution. Contains an inorganic filler having a diameter D50 of 0.5 to 1.0 μm and a particle size D95 at 95% accumulation of 0.9 to 2.0 μm (hereinafter, may be referred to as “inorganic filler A”). It is formed from a thermosetting composition. The thermosetting composition forming the region A can contain a polymerizable compound and a thermal polymerization initiator.
第1の接着剤層2は、導電粒子4(以下、「(A)成分」という場合がある。)、光硬化性樹脂成分(以下、「(B)成分」という場合がある。)の硬化物、及び熱硬化性樹脂成分(以下、「(C)成分」という場合がある。)を含有する。第1の接着剤層2は、例えば、(A)成分、(B)成分、及び(C)成分を含有する組成物からなる組成物層に対して光エネルギーを照射し、(B)成分に含まれる成分を重合させ、(B)成分を硬化させることによって得ることができる。第1の接着剤層2は、(A)成分と、(B)成分の硬化物及び(C)成分を含む接着剤成分5とを含有する。(B)成分の硬化物は、(B)成分を完全に硬化させた硬化物であってもよく、(B)成分の一部を硬化させた硬化物であってもよい。(C)成分は、回路接続時に流動可能な成分であり、例えば、未硬化の硬化性樹脂成分である。 <First adhesive layer>
The first
(A)成分は、導電性を有する粒子であれば特に制限されず、Au、Ag、Pd、Ni、Cu、はんだ等の金属で構成された金属粒子、導電性カーボンで構成された導電性カーボン粒子などであってよい。(A)成分は、非導電性のガラス、セラミック、プラスチック(ポリスチレン等)などを含む核と、上記金属又は導電性カーボンを含み、核を被覆する被覆層とを備える被覆導電粒子であってもよい。これらの中でも、(A)成分は、好ましくは熱溶融性の金属で形成された金属粒子、又はプラスチックを含む核と、金属又は導電性カーボンを含み、核を被覆する被覆層とを備える被覆導電粒子である。このような被覆導電粒子は、熱硬化性樹脂成分の硬化物を加熱又は加圧により変形させることが容易であるため、電極同士を電気的に接続する際に、電極と(A)成分との接触面積を増加させ、電極間の導電性をより向上させることができる。 Component (A): Conductive particles The component (A) is not particularly limited as long as it is a particle having conductivity, and is a metal particle composed of a metal such as Au, Ag, Pd, Ni, Cu, or solder, or conductive carbon. It may be conductive carbon particles composed of. The component (A) may be a coated conductive particle containing a nucleus containing non-conductive glass, ceramic, plastic (polystyrene, etc.) and the like, and a coating layer containing the metal or conductive carbon and covering the nucleus. good. Among these, the component (A) preferably contains metal particles formed of a heat-meltable metal or a core containing plastic, and contains a metal or conductive carbon and has a coating layer covering the core. It is a particle. Since such coated conductive particles can easily deform the cured product of the thermosetting resin component by heating or pressurizing, when the electrodes are electrically connected to each other, the electrode and the component (A) are connected to each other. The contact area can be increased and the conductivity between the electrodes can be further improved.
(B)成分は、光照射によって硬化する樹脂成分であれば特に制限されないが、接続抵抗がより優れる観点から、ラジカル硬化性を有する樹脂成分であってよい。(B)成分は、例えば、ラジカル重合性化合物(以下、「(B1)成分」という場合がある。)及び光ラジカル重合開始剤(以下、「(B2)成分」という場合がある。)を含んでいてもよい。(B)成分は、(B1)成分及び(B2)成分からなる成分であり得る。 Component (B): Photocurable resin component The component (B) is not particularly limited as long as it is a resin component that is cured by light irradiation, but may be a resin component having radical curability from the viewpoint of better connection resistance. .. The component (B) contains, for example, a radically polymerizable compound (hereinafter, may be referred to as “(B1) component”) and a photoradical polymerization initiator (hereinafter, may be referred to as “(B2) component”). You may be. The component (B) can be a component composed of the component (B1) and the component (B2).
(B1)成分は、光(例えば、紫外光)の照射によって(B2)成分から発生したラジカルによって重合する化合物である。(B1)成分は、モノマー、又は、1種若しくは2種以上のモノマーが重合してなるポリマー(又はオリゴマー)のいずれであってもよい。(B1)成分は、1種を単独で用いてもよく、複数を組み合わせて用いてもよい。 Component (B1): Radical Polymerizable Compound The component (B1) is a compound polymerized by radicals generated from the component (B2) by irradiation with light (for example, ultraviolet light). The component (B1) may be either a monomer or a polymer (or oligomer) obtained by polymerizing one or more kinds of monomers. The component (B1) may be used alone or in combination of two or more.
(B2)成分は、150~750nmの範囲内の波長を含む光、好ましくは254~405nmの範囲内の波長を含む光、更に好ましくは365nmの波長を含む光(例えば紫外光)の照射によってラジカルを発生する光重合開始剤である。(B2)成分は、1種を単独で用いてもよく、複数を組み合わせて用いてもよい。 Component (B2): Photoradical Polymerization Initiator The component (B2) comprises light containing a wavelength in the range of 150 to 750 nm, preferably light containing a wavelength in the range of 254 to 405 nm, and more preferably a wavelength in the range of 365 nm. It is a photopolymerization initiator that generates radicals by irradiation with light (for example, ultraviolet light). As the component (B2), one type may be used alone, or a plurality of them may be used in combination.
(C)成分は、例えば、カチオン重合性化合物(以下、「(C1)成分」という場合がある。)及び熱カチオン重合開始剤(以下、「(C2)成分」という場合がある。)を含んでいてもよい。(C)成分は、(C1)成分及び(C2)成分からなる成分であり得る。なお、第1の熱硬化性樹脂成分及び第2の熱硬化性樹脂成分は、それぞれ第1の接着剤層及び第2の接着剤層に含有される熱硬化性樹脂成分を意味する。第1の熱硬化性樹脂成分及び第2の熱硬化性樹脂成分に含まれる成分(例えば、(C1)成分、(C2)成分等)の種類、組み合わせ、及び含有量は、互いに同一であってもよく、異なっていてもよい。 Component (C): Thermosetting resin component The component (C) is, for example, a cationically polymerizable compound (hereinafter, may be referred to as “(C1) component”) and a thermally cationic polymerization initiator (hereinafter, “(C2)). It may be referred to as "ingredient"). The component (C) can be a component composed of the component (C1) and the component (C2). The first thermosetting resin component and the second thermosetting resin component mean the thermosetting resin components contained in the first adhesive layer and the second adhesive layer, respectively. The types, combinations, and contents of the first thermosetting resin component and the components contained in the second thermosetting resin component (for example, (C1) component, (C2) component, etc.) are the same as each other. May be different.
(C1)成分は、熱によって(C2)成分と反応することによって架橋する化合物である。なお、(C1)成分は、ラジカルによって反応するラジカル重合性基を有しない化合物を意味し、(C1)成分は、(B1)成分に包含されない。(C1)成分は、接続抵抗の低減効果が更に向上し、接続信頼性により優れる観点から、分子中に開環重合性の環状エーテル基を1個以上有する化合物であってよい。(C1)成分は、1種を単独で用いてもよく、複数を組み合わせて用いてもよい。分子中に開環重合性の環状エーテル基を1個以上有する化合物としては、例えば、オキセタン化合物及び脂環式エポキシ化合物からなる群より選ばれる少なくとも1種であってよい。(C1)成分は、所望の溶融粘度が得られ易い観点から、オキセタン化合物の少なくとも1種及び脂環式エポキシ化合物の少なくとも1種の両方を含むことが好ましい。 Component (C1): Cationicly polymerizable compound The component (C1) is a compound that crosslinks by reacting with the component (C2) by heat. The component (C1) means a compound having no radically polymerizable group that reacts with a radical, and the component (C1) is not included in the component (B1). The component (C1) may be a compound having one or more ring-opening polymerizable cyclic ether groups in the molecule from the viewpoint of further improving the effect of reducing the connection resistance and improving the connection reliability. The component (C1) may be used alone or in combination of two or more. The compound having one or more ring-opening polymerizable cyclic ether groups in the molecule may be, for example, at least one selected from the group consisting of an oxetane compound and an alicyclic epoxy compound. The component (C1) preferably contains at least one oxetane compound and at least one alicyclic epoxy compound from the viewpoint that the desired melt viscosity can be easily obtained.
(C2)成分は、加熱により酸等を発生して重合を開始する熱重合開始剤である。(C2)成分はカチオンとアニオンとから構成される塩化合物であってよい。(C2)成分は、例えば、BF4 -、BR4 -(Rは、2以上のフッ素原子又は2以上のトリフルオロメチル基で置換されたフェニル基を示す。)、PF6 -、SbF6 -、AsF6 -等のアニオンを有する、スルホニウム塩、ホスホニウム塩、アンモニウム塩、ジアゾニウム塩、ヨードニウム塩、アニリニウム塩等のオニウム塩などが挙げられる。これらは、1種を単独で用いてもよく、複数を組み合わせて用いてもよい。 Component (C2): Thermal Cationic Polymerization Initiator The component (C2) is a thermal polymerization initiator that generates an acid or the like by heating to initiate polymerization. The component (C2) may be a salt compound composed of a cation and an anion. The component (C2) is, for example, BF 4- , BR 4- ( R indicates a phenyl group substituted with 2 or more fluorine atoms or 2 or more trifluoromethyl groups) , PF 6- , SbF 6- . , AsF 6 − and the like, sulfonium salt, phosphonium salt, ammonium salt, diazonium salt, iodonium salt, onium salt such as anilinium salt and the like. These may be used individually by 1 type, and may be used in combination of a plurality of types.
第1の接着剤層2は、(A)成分、(B)成分の硬化物、及び(C)成分以外にその他の成分を更に含有していてもよい。その他の成分としては、例えば、熱可塑性樹脂(以下、「(D)成分」という場合がある。)、カップリング剤(以下、「(E)成分」という場合がある。)、及び、充填材(以下、「(F)成分」という場合がある。)等が挙げられる。 [Other ingredients]
The first
第1の接着剤層2は、軟化剤、促進剤、劣化防止剤、着色剤、難燃化剤、チキソトロピック剤等のその他の添加剤を更に含有していてもよい。その他の添加剤の含有量は、第1の接着剤層の全質量を基準として、例えば、0.1~10質量%であってよい。なお、第1の接着剤層を形成するための組成物又は組成物層中のその他の添加剤の含有量(組成物又は組成物層の全質量基準)は上記範囲と同様であってよい。 [Other additives]
The first
第2の接着剤層3は、(C)成分及び(F)成分を含有することができる。第2の接着剤層3における(C)成分(すなわち、第2の熱硬化性樹脂成分)で使用される(C1)成分及び(C2)成分は、第1の接着剤層2における(C)成分(すなわち、第1の熱硬化性樹脂成分)で使用される(C1)成分及び(C2)成分と同様であることから、ここでは詳細な説明は省略する。第2の熱硬化性樹脂成分は、第1の熱硬化性樹脂成分と同一であっても、異なっていてもよい。 <Second adhesive layer>
The second
(最低溶融粘度の測定方法)
各接着剤フィルムを厚さが200μm以上となるようにラミネータで積層して積層体を得る。得られた積層体から離型処理されたPETを剥離し、10.0mm×10.0mmに切り出して測定試料を得る。得られた測定試料を粘弾性測定装置(商品名:ARES-G2、TAインスツルメンツ社製、昇温速度:10℃/min)を用いて最低溶融粘度を測定する。 The minimum melt viscosity of the
(Measurement method of minimum melt viscosity)
Each adhesive film is laminated with a laminator so as to have a thickness of 200 μm or more to obtain a laminated body. The release-treated PET is peeled off from the obtained laminate and cut into 10.0 mm × 10.0 mm to obtain a measurement sample. The minimum melt viscosity of the obtained measurement sample is measured using a viscoelasticity measuring device (trade name: ARES-G2, manufactured by TA Instruments, Inc., heating rate: 10 ° C./min).
一実施形態の回路接続用接着剤フィルムの製造方法は、例えば、(A)成分、(B)成分、及び(C)成分(第1の熱硬化性樹脂成分)、並びに必要に応じてその他の成分を含有する組成物からなる組成物層に対して光を照射し、第1の接着剤層を形成する工程(第1の工程)と、第1の接着剤層上に、(C)成分(第2の熱硬化性樹脂成分)、及び無機フィラーA、並びに必要に応じてその他の成分を含有する第2の接着剤層を積層する工程(第2の工程)とを備えていてもよい。当該製造方法は、第1の接着剤層の第2の接着剤層とは反対側上に、(C)成分(第3の熱硬化性樹脂成分)、並びに必要に応じて無機フィラーA及びその他の成分を含有する第3の接着剤層を積層する工程(第3の工程)を更に備えていてもよい。この場合、第2の工程を先に行ってもよく、第3の工程を先に行ってもよい。第3の工程を先に行う場合、第1の接着剤層の第2の接着剤層が積層される予定の側とは反対側に第3の接着剤層が積層される。図2は、上記の工程を備える製造方法を示す模式断面図である。 <Manufacturing method of adhesive film for circuit connection>
The method for producing an adhesive film for circuit connection according to one embodiment is, for example, a component (A), a component (B), and a component (C) (first thermosetting resin component), and if necessary, other components. A step of irradiating a composition layer made of a composition containing a component with light to form a first adhesive layer (first step), and a step of forming the component (C) on the first adhesive layer. It may include (second step) of laminating (second thermosetting resin component) and a second adhesive layer containing an inorganic filler A and, if necessary, other components. .. In the manufacturing method, the component (C) (third thermosetting resin component), and if necessary, the inorganic filler A and others are placed on the opposite side of the first adhesive layer from the second adhesive layer. A step of laminating a third adhesive layer containing the above components (third step) may be further provided. In this case, the second step may be performed first, or the third step may be performed first. When the third step is performed first, the third adhesive layer is laminated on the side opposite to the side where the second adhesive layer of the first adhesive layer is to be laminated. FIG. 2 is a schematic cross-sectional view showing a manufacturing method including the above steps.
本実施形態の無機フィラー含有組成物は、体積基準の粒度分布における50%累積時の粒径D50が0.5~1.0μmであり、95%累積時の粒径D95が0.9~2.0μmである無機フィラーを含有する。無機フィラーは、上述した無機フィラーAと同様のものを用いることができる。 <Composition containing inorganic filler>
In the composition containing an inorganic filler of the present embodiment, the particle size D50 at 50% cumulative size is 0.5 to 1.0 μm and the particle size D95 at 95% cumulative size is 0.9 to 2 in the volume-based particle size distribution. Contains an inorganic filler that is 0.0 μm. As the inorganic filler, the same as the above-mentioned inorganic filler A can be used.
以下、回路接続材料として上述の回路接続用接着剤フィルム1aを用いた回路接続構造体及びその製造方法について説明する。 <Circuit connection structure and its manufacturing method>
Hereinafter, a circuit connection structure using the above-mentioned
第1の接着剤層、第2の接着剤層及び第3の接着剤層の作製においては、下記に示す材料を用いた。 [Preparation of First Adhesive Layer, Second Adhesive Layer and Third Adhesive Layer]
In the preparation of the first adhesive layer, the second adhesive layer and the third adhesive layer, the materials shown below were used.
3μmのプラスチック核体の表面に80nmのNiめっきを施し、最表面20nmをPdで置換めっきを施した。このようにして、平均粒径3.2μmの導電粒子を得た。 <Manufacturing of conductive particles>
The surface of a 3 μm plastic nucleus was plated with Ni at 80 nm, and the outermost surface of 20 nm was replaced with Pd. In this way, conductive particles having an average particle size of 3.2 μm were obtained.
A-1:上述のとおり作製した導電粒子 (A) Component: Conductive particles A-1: Conductive particles prepared as described above
(B1)成分:ラジカル重合性化合物
B1-1:NKエステル A-BPEF70T(エトキシ化フルオレン型ジ(メタ)アクリレート(2官能)、新中村化学工業株式会社製)、トルエンで不揮発分70質量%に希釈したものを使用
B1-2:リポキシ VR-90(ビスフェノールA型エポキシ(メタ)アクリレート(2官能)(ビニルエステル樹脂)、昭和電工株式会社製) (B) component: Photocurable resin component (B1) component: Radical polymerizable compound B1-1: NK ester A-BPEF70T (ethoxylated fluorene type di (meth) acrylate (bifunctional), manufactured by Shin-Nakamura Chemical Industry Co., Ltd.) ), Diluted with toluene to 70% by mass of non-volatile content B1-2: Lipoxy VR-90 (bisphenol A type epoxy (meth) acrylate (bifunctional) (vinyl ester resin), manufactured by Showa Denko Co., Ltd.)
B2-1:Irgacure OXE-02(エタノン,1-[9-エチル-6-(2-メチルベンゾイル)-9H-カルバゾール-3-イル]-,1-(0-アセチルオキシム)、BASF社製)、MEKで不揮発分10質量%に希釈したものを使用 (B2) Ingredients: Photoradical Polymerization Initiator B2-1: Acetyl OXE-02 (Etanon, 1- [9-ethyl-6- (2-methylbenzoyl) -9H-carbazole-3-yl]-, 1-( 0-Acetyl oxime), manufactured by BASF), MEK diluted to 10% by mass of non-volatile content
(C1)成分:カチオン重合性化合物
C1-1:ETERNACOLL OXBP(3-エチル-3-ヒドロキシメチルオキセタン、宇部興産株式会社製)
C1-2:EHPE3150(2,2-ビス(ヒドロキシメチル)-1-ブタノールの1,2-エポキシ-4-(2-オキシラニル)シクロヘキサン付加物、株式会社ダイセル製)
C1-3:セロキサイド2021P(3,4-エポキシシクロヘキシルメチル(3, 4-エポキシ)シクロヘキサンカロボキシレート、株式会社ダイセル製)
C1-4:OXSQ-TX100(ポリ({3-[(3-エチル-3-オキセタニル)メトキシ]プロピル}シルセスキオキサン)誘導体、東亜合成株式会社製)
C1-5:セロキサイド8010(ビ-7-オキサビシクロ[4.1.0]ヘプタン、株式会社ダイセル製) (C) component: Thermosetting resin component (C1) component: Cationic polymerizable compound C1-1: ETERNACOLL OXBP (3-ethyl-3-hydroxymethyloxetane, manufactured by Ube Industries, Ltd.)
C1-2: EHPE3150 (1,2-epoxy-4- (2-oxylanyl) cyclohexane adduct of 2,2-bis (hydroxymethyl) -1-butanol, manufactured by Daicel Corporation)
C1-3: Celoxide 2021P (3,4-epoxycyclohexylmethyl (3,4-epoxy) cyclohexanecarboxylate, manufactured by Daicel Corporation)
C1-4: OXSQ-TX100 (poly ({3-[(3-ethyl-3-oxetanyl) methoxy] propyl} silsesquioxane) derivative, manufactured by Toagosei Corporation)
C1-5: Celoxide 8010 (B-7-oxavicyclo [4.1.0] heptane, manufactured by Daicel Corporation)
C2-1:CXC-1821(King Industries社製) (C2) Ingredient: Thermal Cationic Polymerization Initiator C2-1: CXC-1821 (manufactured by King Industries)
D-1:フェノトート YP-50S(ビスフェノールA型フェノキシ樹脂、重量平均分子量:60,000、ガラス転移温度:84℃、日鉄ケミカル&マテリアル株式会社製)、MEKで不揮発分40質量%に希釈したものを使用
D-2:TOPR-300(高Tgタイプエポキシ樹脂、エポキシ当量:900~1,000、軟化点:120℃、日鉄ケミカル&マテリアル株式会社製)、MEKで不揮発分60質量%に希釈したものを使用
D-3:フェノトート FX-293(フルオレン骨格含有フェノキシ樹脂、重量平均分子量:45,000、ガラス転移温度:158℃、日鉄ケミカル&マテリアル株式会社製)、MEKで不揮発分60質量%に希釈したものを使用
D-4:フェノトート ZX-1356-2(ビスフェノールA型及びビスフェノールF型の共重合型フェノキシ樹脂、重量平均分子量:70000、ガラス転移温度:71℃、日鉄ケミカル&マテリアル株式会社製)、MEKで不揮発分40質量%に希釈したものを使用 (D) Ingredients: Epoxy resin D-1: Phenototo YP-50S (bisphenol A type phenoxy resin, weight average molecular weight: 60,000, glass transition temperature: 84 ° C., manufactured by Nittetsu Chemical & Materials Co., Ltd.), MEK D-2: TOPR-300 (high Tg type epoxy resin, epoxy equivalent: 900-1,000, softening point: 120 ° C, manufactured by Nittetsu Chemical & Materials Co., Ltd.) D-3: Phenototo FX-293 (fluorene skeleton-containing phenoxy resin, weight average molecular weight: 45,000, glass transition temperature: 158 ° C, Nittetsu Chemical & Materials Made by MEK, diluted to 60% by mass of non-volatile content D-4: Phenototo ZX-1356-2 (bisphenol A type and bisphenol F type copolymer phenoxy resin, weight average molecular weight: 70000, Glass transition temperature: 71 ° C, manufactured by Nittetsu Chemical & Materials Co., Ltd.), using MEK diluted to 40% by mass of non-volatile content
E-1:SH-6040(3-グリシドキシプロピルトリメトキシシラン、東レ・ダウコーニング株式会社製) (E) Ingredient: Coupling agent E-1: SH-6040 (3-glycidoxypropyltrimethoxysilane, manufactured by Toray Dow Corning Co., Ltd.)
(F1)成分:無機フィラー
F-1:アドマファインSE2050(シリカフィラー、株式会社アドマテックス製)、風力分級によって1μm以上の粒子をできるだけカットした後、MEKで不揮発分70質量%に希釈したものを使用
F-2:アドマファインSE2050(シリカフィラー、株式会社アドマテックス製)、MEKで不揮発分70質量%に希釈したものを使用
F-3:アドマナノYA050C(シリカフィラー、株式会社アドマテックス製)、MEKで不揮発分50質量%に希釈したものを使用
F-4:アエロジルR805(シリカフィラー、Evonik Industries AG製)、MEKで不揮発分10質量%に希釈したものを使用 (F) Component: Filler (F1) Component: Inorganic filler F-1: Admafine SE2050 (silica filler, manufactured by Admatex Co., Ltd.), after cutting particles of 1 μm or more as much as possible by wind classification, non-volatile content 70 with MEK F-2: Admafine SE2050 (silica filler, manufactured by Admatex Co., Ltd.), diluted to 70% by mass of non-volatile content with MEK F-3: Admanano YA050C (silica filler, stock) (Manufactured by Admatex), use MEK diluted to 50% by mass of non-volatile content F-4: Aerosil R805 (silica filler, manufactured by Evonik Industries AG), use MEK diluted to 10% by mass of non-volatile content
上記無機フィラーの体積基準の粒度分布における50%累積時の粒径D50(累積分布50体積%の粒径)及び95%累積時の粒径D95(累積分布95体積%の粒径)を測定した。測定には、測定装置として日機装株式会社製のMicrotorac MT3300EXIIを用い、測定溶媒としてメチルエチルケトンを用いた。 <Measurement of particle size distribution of inorganic filler-1>
In the volume-based particle size distribution of the inorganic filler, the particle size D50 at the time of 50% accumulation (particle size of the cumulative distribution 50% by volume) and the particle size D95 at the time of 95% accumulation (particle size of the cumulative distribution 95% by volume) were measured. .. For the measurement, Microtorac MT3300EXII manufactured by Nikkiso Co., Ltd. was used as a measuring device, and methyl ethyl ketone was used as a measuring solvent.
表2に示す材料を表2に示す組成比(質量比)(表2の数値は不揮発分量を意味する。)で混合した組成物を得た後、離型処理されたPET(ポリエチレンテレフタレート)フィルムの上に磁場を掛けながら塗工し、有機溶媒等を70℃で5分間熱風乾燥することによって、各成分を含有する組成物からなる組成物層をそれぞれ得た。組成物層は、乾燥後の厚さがそれぞれ3~4μmとなるように塗工した。その後、組成物層に対してそれぞれ光照射することによって(UV照射:メタルハライドランプ、積算光量:2100mJ/cm2)、導電粒子が分散した第1の接着剤層を作製した。ここでの厚さは接触式厚み計を用いて測定した。 <Preparation of the first adhesive layer>
A PET (polyethylene terephthalate) film obtained by mixing the materials shown in Table 2 with the composition ratio (mass ratio) shown in Table 2 (the numerical values in Table 2 mean the non-volatile content) and then performing a mold release treatment. A composition layer composed of a composition containing each component was obtained by applying the coating on the above while applying a magnetic field and drying the organic solvent or the like at 70 ° C. for 5 minutes with hot air. The composition layer was coated so that the thickness after drying was 3 to 4 μm, respectively. Then, by irradiating each of the composition layers with light (UV irradiation: metal halide lamp, integrated light amount: 2100 mJ / cm 2 ), a first adhesive layer in which conductive particles were dispersed was prepared. The thickness here was measured using a contact thickness gauge.
表3に示す材料を表3に示す組成比(質量比)(表3の数値は不揮発分量を意味する。)で混合した組成物を得た後、離型処理されたPET(ポリエチレンテレフタレート)フィルムの上に塗工し、有機溶媒等を70℃で5分間熱風乾燥することによって、各成分を含有する組成物からなる第2の接着剤層をそれぞれ作製した。接着剤層は、乾燥後の厚さがそれぞれ8~9μmとなるように塗工した。ここでの厚さは接触式厚み計を用いて測定した。 <Preparation of second adhesive layer>
A PET (polyethylene terephthalate) film obtained by mixing the materials shown in Table 3 with the composition ratio (mass ratio) shown in Table 3 (the numerical values in Table 3 mean the non-volatile content) and then performing a mold release treatment. A second adhesive layer composed of a composition containing each component was prepared by coating on the above and drying an organic solvent or the like at 70 ° C. for 5 minutes with hot air. The adhesive layer was coated so that the thickness after drying was 8 to 9 μm, respectively. The thickness here was measured using a contact thickness gauge.
第2の接着剤層を形成する際の塗工歩留まりについて、白線及びスクラッチが発生しない割合Y(%)を求め、下記の基準で評価した。
A+:Yが95%以上である
A:Yが90%以上95%未満である
B:Yが80%以上90%未満である
C:Yが80%未満である (Coating yield)
Regarding the coating yield when forming the second adhesive layer, the ratio Y (%) at which white lines and scratches did not occur was determined and evaluated according to the following criteria.
A +: Y is 95% or more A: Y is 90% or more and less than 95% B: Y is 80% or more and less than 90% C: Y is less than 80%
組成物S1-4に含まれる無機フィラー(80質量部のF-1及び5質量部のF-3の混合物)について、上記と同様にして体積基準の粒度分布における50%累積時の粒径D50(累積分布50体積%の粒径)及び95%累積時の粒径D95(累積分布95体積%の粒径)を測定した。 <Measurement of particle size distribution of inorganic filler-2>
For the inorganic filler (a mixture of 80 parts by mass F-1 and 5 parts by mass F-3) contained in the composition S1-4, the particle size D50 at the time of 50% accumulation in the volume-based particle size distribution in the same manner as above. (Particulate particle size of cumulative distribution 50% by volume) and particle size D95 at the time of 95% accumulation (particle size of cumulative distribution 95% by volume) were measured.
表5に示す材料を表5に示す組成比(質量比)(表5の数値は不揮発分量を意味する。)で混合した組成物を得た後、離型処理されたPET(ポリエチレンテレフタレート)フィルムの上に塗工し、有機溶媒等を70℃で5分間熱風乾燥することによって、各成分を含有する組成物からなる第3の接着剤層を製した。接着剤層は、乾燥後の厚さがそれぞれ0.5~1.5μmとなるように塗工した。ここでの厚さは接触式厚み計を用いて測定した。 <Preparation of third adhesive layer>
A PET (polyethylene terephthalate) film obtained by mixing the materials shown in Table 5 with the composition ratio (mass ratio) shown in Table 5 (the numerical values in Table 5 mean the non-volatile content) and then performing a mold release treatment. A third adhesive layer made of a composition containing each component was prepared by coating on the above and drying an organic solvent or the like at 70 ° C. for 5 minutes with hot air. The adhesive layer was coated so that the thickness after drying was 0.5 to 1.5 μm, respectively. The thickness here was measured using a contact thickness gauge.
[接着剤フィルムの作製]
上記で作製した第1の接着剤層、第2の接着剤層及び第3の接着剤層を用いて、表6に示す構成の接着剤フィルムを作製した。例えば、実施例1の接着剤フィルムにおいては、組成物S1-1によって形成した第2の接着剤層に、組成物P-1によって形成した第1の接着剤層を50~60℃の温度をかけながら張り合わせ、第1の接着剤層側のPETフィルムを剥がした。次に、露出した第1の接着剤層に、組成物S2-1によって形成した第3の接着剤層を50~60℃の温度をかけながら張り合わせて、実施例1の接着剤フィルムを得た。なお、これらの一連の工程において剥離するPETフィルム及び回路接続の際に剥離するPETフィルムを剥がしやすくするために、第2の接着剤層とPETフィルムとの間の剥離力が、第1の接着剤層とPETフィルムとの間の剥離力及び第3の接着剤層とPETフィルムとの間の剥離力よりも大きくなるように、各PETフィルムを選定した。 (Examples 1 to 5 and Comparative Examples 1 to 5)
[Preparation of adhesive film]
Using the first adhesive layer, the second adhesive layer, and the third adhesive layer prepared above, an adhesive film having the constitution shown in Table 6 was prepared. For example, in the adhesive film of Example 1, the first adhesive layer formed by the composition P-1 is heated to a temperature of 50 to 60 ° C. on the second adhesive layer formed by the composition S1-1. The PET film on the first adhesive layer side was peeled off. Next, the third adhesive layer formed by the composition S2-1 was bonded to the exposed first adhesive layer while applying a temperature of 50 to 60 ° C. to obtain the adhesive film of Example 1. .. In order to facilitate the peeling of the PET film that is peeled off in these series of steps and the PET film that is peeled off at the time of circuit connection, the peeling force between the second adhesive layer and the PET film is the first adhesion. Each PET film was selected so as to be larger than the peeling force between the agent layer and the PET film and the peeling force between the third adhesive layer and the PET film.
<回路接続構造体-1の作製>
第1の回路部材として、バンプ電極を2列で千鳥状に配列したICチップ(0.9mm×20.3mm、厚さ:0.3mm、バンプ電極の大きさ:70μm×12μm、バンプ電極間スペース:12μm、バンプ電極厚さ:9μm)を準備した。また、第2の回路部材として、ポリイミド基板(東レ・デュポン株式会社製、200H)(38mm×28mm、厚さ:0.05mm)の表面に、Ti:50nm/Al:400nmの配線パターン(パターン幅:19μm、電極間スペース:5μm)を形成したものを準備した。 [Evaluation of circuit connection structure]
<Manufacturing of circuit connection structure-1>
As the first circuit member, an IC chip (0.9 mm × 20.3 mm, thickness: 0.3 mm, bump electrode size: 70 μm × 12 μm, space between bump electrodes) in which bump electrodes are arranged in two rows in a staggered pattern. : 12 μm, bump electrode thickness: 9 μm) was prepared. Further, as a second circuit member, a wiring pattern (pattern width) of Ti: 50 nm / Al: 400 nm is provided on the surface of a polyimide substrate (manufactured by Toray DuPont Co., Ltd., 200H) (38 mm × 28 mm, thickness: 0.05 mm). : 19 μm, space between electrodes: 5 μm) was prepared.
第1の回路部材として、バンプ電極を2列で千鳥状に配列したICチップ(0.9mm×20.3mm、厚さ:0.3mm、バンプ電極の大きさ:70μm×12μm、バンプ電極間スペース:12μm、バンプ電極厚さ:5μm)を準備した。また、第2の回路部材として、ガラス基板(25mm×35mm、厚さ:0.2mm)の表面に、150nm厚みのAl/Ndを成膜したものを準備した。 <Manufacturing of circuit connection structure-2>
As the first circuit member, an IC chip (0.9 mm × 20.3 mm, thickness: 0.3 mm, bump electrode size: 70 μm × 12 μm, space between bump electrodes) in which bump electrodes are arranged in two rows in a staggered pattern. : 12 μm, bump electrode thickness: 5 μm) was prepared. Further, as a second circuit member, a glass substrate (25 mm × 35 mm, thickness: 0.2 mm) having an Al / Nd film having a thickness of 150 nm was prepared on the surface of the glass substrate (25 mm × 35 mm, thickness: 0.2 mm).
作製した回路接続構造体-1について、初期の接続抵抗(導通抵抗)を4端子法によって測定した。測定には、楠本化成株式会社製のマルチメータMLR21を用いた。電位差を任意の14点で測定し、その平均値を求めた。電位差の平均値を接続抵抗値に換算し、下記の基準で評価した。結果を表6に示す。
A:接続抵抗値が0.6Ω未満
B:接続抵抗値が0.6Ω以上1.0Ω未満
C:接続抵抗値が1.0Ω以上 (Evaluation of connection resistance)
The initial connection resistance (conduction resistance) of the produced circuit connection structure-1 was measured by the 4-terminal method. A multimeter MLR21 manufactured by Kusumoto Kasei Co., Ltd. was used for the measurement. The potential difference was measured at any 14 points, and the average value was obtained. The average value of the potential difference was converted into the connection resistance value and evaluated according to the following criteria. The results are shown in Table 6.
A: Connection resistance value is less than 0.6Ω B: Connection resistance value is 0.6Ω or more and less than 1.0Ω C: Connection resistance value is 1.0Ω or more
作製した回路接続構造体-2を、微分干渉顕微鏡を用いてガラス基板側から観察することにより、導電粒子の圧痕よりも明らかに強い(視覚的に目立つ)圧痕(大圧痕)の有無を確認し、このような大圧痕が見られない場合を「A」、見られる場合を「B」として評価した。 (Evaluation of large indentations)
By observing the produced circuit connection structure-2 from the glass substrate side using a differential interference microscope, it was confirmed whether or not there were indentations (large indentations) that were clearly stronger (visually conspicuous) than the indentations of the conductive particles. , The case where such a large indentation was not seen was evaluated as "A", and the case where such a large indentation was seen was evaluated as "B".
表7に示す材料を表7に示す組成比(質量比)(表7の数値は不揮発分量を意味する。)で混合した組成物を得た後、離型処理されたPET(ポリエチレンテレフタレート)フィルムの上に塗工し、有機溶媒等を70℃で5分間熱風乾燥することによって、各成分を含有する組成物からなる組成物層をそれぞれ得た。組成物層は、乾燥後の厚さが5μmとなるように塗工し、第1の接着剤層-Bを作製した。ここでの厚さは接触式厚み計を用いて測定した。 <Preparation of the first adhesive layer-B>
A PET (polyethylene terephthalate) film obtained by mixing the materials shown in Table 7 with the composition ratio (mass ratio) shown in Table 7 (the numerical values in Table 7 mean the non-volatile content) and then performing a mold release treatment. A composition layer composed of a composition containing each component was obtained by coating on the above and drying an organic solvent or the like at 70 ° C. for 5 minutes with hot air. The composition layer was coated so as to have a thickness of 5 μm after drying to prepare a first adhesive layer-B. The thickness here was measured using a contact thickness gauge.
表8に示す材料を表8に示す組成比(質量比)(表8の数値は不揮発分量を意味する。)で混合した組成物を得た後、離型処理されたPET(ポリエチレンテレフタレート)フィルムの上に塗工し、有機溶媒等を70℃で5分間熱風乾燥することによって、各成分を含有する組成物からなる第2の接着剤層-Bをそれぞれ作製した。接着剤層は、乾燥後の厚さがそれぞれ11μmとなるように塗工した。ここでの厚さは接触式厚み計を用いて測定した。 <Preparation of the second adhesive layer-B>
A PET (polyethylene terephthalate) film obtained by mixing the materials shown in Table 8 with the composition ratio (mass ratio) shown in Table 8 (the numerical values in Table 8 mean the non-volatile content) and then performing a mold release treatment. A second adhesive layer-B made of a composition containing each component was prepared by coating on the above and drying an organic solvent or the like at 70 ° C. for 5 minutes with hot air. The adhesive layer was coated so that the thickness after drying was 11 μm each. The thickness here was measured using a contact thickness gauge.
第2の接着剤層-Bを形成する際の塗工歩留まりについて、白線及びスクラッチが発生しない割合Y(%)を求め、下記の基準で評価した。
A+:Yが95%以上である
A:Yが90%以上95%未満である
B:Yが80%以上90%未満である
C:Yが80%未満である (Coating yield)
Regarding the coating yield when forming the second adhesive layer-B, the ratio Y (%) at which white lines and scratches did not occur was determined and evaluated according to the following criteria.
A +: Y is 95% or more A: Y is 90% or more and less than 95% B: Y is 80% or more and less than 90% C: Y is less than 80%
[接着剤フィルムの作製]
上記で作製した第1の接着剤層-B及び第2の接着剤層-Bを用いて、表9に示す構成の接着剤フィルムを作製した。例えば、実施例6の接着剤フィルムにおいては、組成物S1-9によって形成した第2の接着剤層-Bに、組成物P-2によって形成した第1の接着剤層-Bを50~60℃の温度をかけながら張り合わせ、実施例6の接着剤フィルムを得た。 (Example 6 and Comparative Examples 6 to 8)
[Preparation of adhesive film]
Using the first adhesive layer-B and the second adhesive layer-B prepared above, an adhesive film having the constitution shown in Table 9 was prepared. For example, in the adhesive film of Example 6, 50 to 60 first adhesive layers-B formed by the composition P-2 are added to the second adhesive layer-B formed by the composition S1-9. The adhesive film of Example 6 was obtained by laminating while applying a temperature of ° C.
第1の回路部材として、バンプ電極を2列で千鳥状に配列したICチップ(0.9mm×20.3mm、厚さ:0.3mm、バンプ電極の大きさ:70μm×12μm、バンプ電極間スペース:12μm、バンプ電極厚さ:5μm)を準備した。また、第2の回路部材として、ガラス基板(25mm×35mm、厚さ:0.2mm)の表面に、150nm厚みのTi/Al/Tiを成膜したものを準備した。 <Manufacturing of circuit connection structure-3>
As the first circuit member, an IC chip (0.9 mm × 20.3 mm, thickness: 0.3 mm, bump electrode size: 70 μm × 12 μm, space between bump electrodes) in which bump electrodes are arranged in two rows in a staggered pattern. : 12 μm, bump electrode thickness: 5 μm) was prepared. Further, as a second circuit member, a glass substrate (25 mm × 35 mm, thickness: 0.2 mm) having a Ti / Al / Ti film having a thickness of 150 nm was prepared on the surface of the glass substrate (25 mm × 35 mm, thickness: 0.2 mm).
作製した回路接続構造体-3について、初期の接続抵抗(導通抵抗)を4端子法によって測定した。測定には、楠本化成株式会社製のマルチメータMLR21を用いた。電位差を任意の14点で測定し、その平均値を求めた。電位差の平均値を接続抵抗値に換算し、下記の基準で評価した。結果を表9に示す。
A:接続抵抗値が5Ω未満
B:接続抵抗値が5Ω以上10Ω未満
C:接続抵抗値が10Ω以上 (Evaluation of connection resistance)
The initial connection resistance (conduction resistance) of the produced circuit connection structure-3 was measured by the 4-terminal method. A multimeter MLR21 manufactured by Kusumoto Kasei Co., Ltd. was used for the measurement. The potential difference was measured at any 14 points, and the average value was obtained. The average value of the potential difference was converted into the connection resistance value and evaluated according to the following criteria. The results are shown in Table 9.
A: Connection resistance value is less than 5Ω B: Connection resistance value is 5Ω or more and less than 10Ω C: Connection resistance value is 10Ω or more
作製した回路接続構造体-3を、微分干渉顕微鏡を用いてガラス基板側から観察することにより、導電粒子の圧痕よりも明らかに強い(視覚的に目立つ)圧痕(大圧痕)の有無を確認し、このような大圧痕が見られない場合を「A」、見られる場合を「B」として評価した。 (Evaluation of large indentations)
By observing the produced circuit connection structure-3 from the glass substrate side using a differential interference microscope, it was confirmed whether or not there were indentations (large indentations) that were clearly stronger (visually conspicuous) than the indentations of the conductive particles. , The case where such a large indentation was not seen was evaluated as "A", and the case where such a large indentation was seen was evaluated as "B".
Claims (14)
- 導電粒子を含む回路接続用接着剤フィルムであって、
前記接着剤フィルムは、フィルムの厚さ方向において、無機フィラーを含有する領域Aを含み、
前記領域Aは、体積基準の粒度分布における50%累積時の粒径D50が0.5~1.0μmであり、95%累積時の粒径D95が0.9~2.0μmである無機フィラーを含有する熱硬化性組成物から形成されている、回路接続用接着剤フィルム。 An adhesive film for circuit connection containing conductive particles.
The adhesive film contains a region A containing an inorganic filler in the thickness direction of the film.
In the region A, the particle size D50 at the time of 50% accumulation is 0.5 to 1.0 μm and the particle size D95 at the time of 95% accumulation is 0.9 to 2.0 μm in the volume-based particle size distribution. An adhesive film for circuit connection, which is formed from a thermosetting composition containing. - 前記接着剤フィルムが、フィルムの厚さ方向において、導電粒子を含まない領域Sを含み、
前記領域Aが前記領域Sの少なくとも一部に設けられている、請求項1に記載の回路接続用接着剤フィルム。 The adhesive film contains a region S that does not contain conductive particles in the thickness direction of the film.
The circuit connection adhesive film according to claim 1, wherein the region A is provided in at least a part of the region S. - 前記無機フィラーが、シリカフィラーである、請求項1又は2に記載の回路接続用接着剤フィルム。 The circuit connection adhesive film according to claim 1 or 2, wherein the inorganic filler is a silica filler.
- 導電粒子、光硬化性樹脂成分の硬化物、及び第1の熱硬化性樹脂成分を含有する第1の接着剤層と、第1の接着剤層上に設けられた、第2の熱硬化性樹脂成分を含有する第2の接着剤層とを備え、
前記第2の接着剤層は、前記第2の熱硬化性樹脂成分と、体積基準の粒度分布における50%累積時の粒径D50が0.5~1.0μmであり、95%累積時の粒径D95が0.9~2.0μmである無機フィラーと、を含有する無機フィラー含有組成物からなる、回路接続用接着剤フィルム。 A first adhesive layer containing conductive particles, a cured product of a photocurable resin component, and a first thermosetting resin component, and a second thermosetting layer provided on the first adhesive layer. With a second adhesive layer containing a resin component,
The second adhesive layer has a particle size D50 of the second thermosetting resin component and a particle size D50 at 50% cumulative in a volume-based particle size distribution of 0.5 to 1.0 μm, and has a particle size D50 at 95% cumulative. An adhesive film for circuit connection comprising an inorganic filler having a particle size D95 of 0.9 to 2.0 μm and an inorganic filler-containing composition containing the inorganic filler. - 前記無機フィラーが、シリカフィラーである、請求項4に記載の回路接続用接着剤フィルム。 The circuit connection adhesive film according to claim 4, wherein the inorganic filler is a silica filler.
- 前記第1の接着剤層の前記第2の接着剤層とは反対側上に積層された、第3の熱硬化性樹脂成分を含む第3の接着剤層を更に備える、請求項4又は5に記載の回路接続用接着剤フィルム。 4 or 5 further comprising a third adhesive layer containing a third thermosetting resin component laminated on the opposite side of the first adhesive layer from the second adhesive layer. Adhesive film for circuit connection described in.
- 導電粒子及び無機フィラーを含有する回路接続用部材における無機フィラー含有領域を形成するために用いられる組成物であって、
体積基準の粒度分布における50%累積時の粒径D50が0.5~1.0μmであり、95%累積時の粒径D95が0.9~2.0μmである無機フィラーを含有する、無機フィラー含有組成物。 A composition used for forming an inorganic filler-containing region in a circuit connection member containing conductive particles and an inorganic filler.
Inorganic filler containing an inorganic filler having a 50% cumulative particle size D50 of 0.5 to 1.0 μm and a 95% cumulative particle size D95 of 0.9 to 2.0 μm in a volume-based particle size distribution. Filler-containing composition. - 前記無機フィラーが、シリカフィラーである、請求項7に記載の無機フィラー含有組成物。 The inorganic filler-containing composition according to claim 7, wherein the inorganic filler is a silica filler.
- 熱可塑性樹脂を更に含有する、請求項7又は8に記載の無機フィラー含有組成物。 The inorganic filler-containing composition according to claim 7 or 8, further containing a thermoplastic resin.
- 厚みが10μm以下の接着剤層を形成するために用いられる、請求項7~9のいずれか一項に記載の無機フィラー含有組成物。 The inorganic filler-containing composition according to any one of claims 7 to 9, which is used for forming an adhesive layer having a thickness of 10 μm or less.
- 第1の電極を有する第1の回路部材と、第2の電極を有する第2の回路部材との間に、請求項1~6のいずれか一項に記載の回路接続用接着剤フィルムを介在させ、前記第1の回路部材及び前記第2の回路部材を熱圧着して、前記第1の電極及び前記第2の電極を互いに電気的に接続する工程を備える、回路接続構造体の製造方法。 The circuit connection adhesive film according to any one of claims 1 to 6 is interposed between a first circuit member having a first electrode and a second circuit member having a second electrode. A method for manufacturing a circuit connection structure, comprising a step of thermally crimping the first circuit member and the second circuit member to electrically connect the first electrode and the second electrode to each other. ..
- 前記第1の回路部材及び前記第2の回路部材のうちの一方がICチップであり、他方がTiを含む電極を有するプラスチック基板である、請求項11に記載の回路接続構造体の製造方法。 The method for manufacturing a circuit connection structure according to claim 11, wherein one of the first circuit member and the second circuit member is an IC chip and the other is a plastic substrate having an electrode containing Ti.
- 第1の電極を有する第1の回路部材と、
第2の電極を有する第2の回路部材と、
前記第1の回路部材及び前記第2の回路部材の間に配置され、前記第1の電極及び前記第2の電極を互いに電気的に接続する回路接続部と、
を備え、
前記回路接続部が、請求項1~6のいずれか一項に記載の回路接続用接着剤フィルムの硬化物を含む、回路接続構造体。 A first circuit member having a first electrode and
A second circuit member having a second electrode and
A circuit connection portion that is arranged between the first circuit member and the second circuit member and electrically connects the first electrode and the second electrode to each other.
Equipped with
A circuit connection structure in which the circuit connection portion contains a cured product of the adhesive film for circuit connection according to any one of claims 1 to 6. - 前記第1の回路部材及び前記第2の回路部材のうちの一方がICチップであり、他方がTiを含む電極を有するプラスチック基板である、請求項13に記載の回路接続構造体。 The circuit connection structure according to claim 13, wherein one of the first circuit member and the second circuit member is an IC chip and the other is a plastic substrate having an electrode containing Ti.
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