WO2023008186A1 - 接着性樹脂シート、プリント配線板および、電子機器 - Google Patents
接着性樹脂シート、プリント配線板および、電子機器 Download PDFInfo
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- WO2023008186A1 WO2023008186A1 PCT/JP2022/027466 JP2022027466W WO2023008186A1 WO 2023008186 A1 WO2023008186 A1 WO 2023008186A1 JP 2022027466 W JP2022027466 W JP 2022027466W WO 2023008186 A1 WO2023008186 A1 WO 2023008186A1
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- 239000000395 magnesium oxide Substances 0.000 description 1
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 1
- 229910052943 magnesium sulfate Inorganic materials 0.000 description 1
- 235000019341 magnesium sulphate Nutrition 0.000 description 1
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 description 1
- 230000007257 malfunction Effects 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- ZQKXQUJXLSSJCH-UHFFFAOYSA-N melamine cyanurate Chemical compound NC1=NC(N)=NC(N)=N1.O=C1NC(=O)NC(=O)N1 ZQKXQUJXLSSJCH-UHFFFAOYSA-N 0.000 description 1
- YSRVJVDFHZYRPA-UHFFFAOYSA-N melem Chemical compound NC1=NC(N23)=NC(N)=NC2=NC(N)=NC3=N1 YSRVJVDFHZYRPA-UHFFFAOYSA-N 0.000 description 1
- 108091063785 miR-3000 stem-loop Proteins 0.000 description 1
- 239000010445 mica Substances 0.000 description 1
- 229910052618 mica group Inorganic materials 0.000 description 1
- 239000012046 mixed solvent Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910000476 molybdenum oxide Inorganic materials 0.000 description 1
- 239000000178 monomer Substances 0.000 description 1
- IJUDHTPONBSVRJ-UHFFFAOYSA-N n-[2-[[5-(dimethylamino)naphthalen-1-yl]sulfonylamino]ethyl]-3,5-bis(2,5-dioxopyrrol-1-yl)benzamide Chemical compound C1=CC=C2C(N(C)C)=CC=CC2=C1S(=O)(=O)NCCNC(=O)C(C=1)=CC(N2C(C=CC2=O)=O)=CC=1N1C(=O)C=CC1=O IJUDHTPONBSVRJ-UHFFFAOYSA-N 0.000 description 1
- GKTNLYAAZKKMTQ-UHFFFAOYSA-N n-[bis(dimethylamino)phosphinimyl]-n-methylmethanamine Chemical class CN(C)P(=N)(N(C)C)N(C)C GKTNLYAAZKKMTQ-UHFFFAOYSA-N 0.000 description 1
- HNHVTXYLRVGMHD-UHFFFAOYSA-N n-butyl isocyanate Chemical compound CCCCN=C=O HNHVTXYLRVGMHD-UHFFFAOYSA-N 0.000 description 1
- 125000001624 naphthyl group Chemical group 0.000 description 1
- 229910000480 nickel oxide Inorganic materials 0.000 description 1
- KQJBQMSCFSJABN-UHFFFAOYSA-N octadecan-1-olate;titanium(4+) Chemical compound [Ti+4].CCCCCCCCCCCCCCCCCC[O-].CCCCCCCCCCCCCCCCCC[O-].CCCCCCCCCCCCCCCCCC[O-].CCCCCCCCCCCCCCCCCC[O-] KQJBQMSCFSJABN-UHFFFAOYSA-N 0.000 description 1
- VRQWWCJWSIOWHG-UHFFFAOYSA-J octadecanoate;zirconium(4+) Chemical compound [Zr+4].CCCCCCCCCCCCCCCCCC([O-])=O.CCCCCCCCCCCCCCCCCC([O-])=O.CCCCCCCCCCCCCCCCCC([O-])=O.CCCCCCCCCCCCCCCCCC([O-])=O VRQWWCJWSIOWHG-UHFFFAOYSA-J 0.000 description 1
- MCCIMQKMMBVWHO-UHFFFAOYSA-N octadecanoic acid;titanium Chemical compound [Ti].CCCCCCCCCCCCCCCCCC(O)=O.CCCCCCCCCCCCCCCCCC(O)=O.CCCCCCCCCCCCCCCCCC(O)=O.CCCCCCCCCCCCCCCCCC(O)=O MCCIMQKMMBVWHO-UHFFFAOYSA-N 0.000 description 1
- KSCKTBJJRVPGKM-UHFFFAOYSA-N octan-1-olate;titanium(4+) Chemical compound [Ti+4].CCCCCCCC[O-].CCCCCCCC[O-].CCCCCCCC[O-].CCCCCCCC[O-] KSCKTBJJRVPGKM-UHFFFAOYSA-N 0.000 description 1
- 238000010943 off-gassing Methods 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- MPQXHAGKBWFSNV-UHFFFAOYSA-N oxidophosphanium Chemical class [PH3]=O MPQXHAGKBWFSNV-UHFFFAOYSA-N 0.000 description 1
- 150000002923 oximes Chemical class 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- VTRUBDSFZJNXHI-UHFFFAOYSA-N oxoantimony Chemical compound [Sb]=O VTRUBDSFZJNXHI-UHFFFAOYSA-N 0.000 description 1
- PQQKPALAQIIWST-UHFFFAOYSA-N oxomolybdenum Chemical compound [Mo]=O PQQKPALAQIIWST-UHFFFAOYSA-N 0.000 description 1
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 1
- 150000002989 phenols Chemical class 0.000 description 1
- 125000000951 phenoxy group Chemical group [H]C1=C([H])C([H])=C(O*)C([H])=C1[H] 0.000 description 1
- NAKOELLGRBLZOF-UHFFFAOYSA-N phenoxybenzene;pyrrole-2,5-dione Chemical compound O=C1NC(=O)C=C1.O=C1NC(=O)C=C1.C=1C=CC=CC=1OC1=CC=CC=C1 NAKOELLGRBLZOF-UHFFFAOYSA-N 0.000 description 1
- DGTNSSLYPYDJGL-UHFFFAOYSA-N phenyl isocyanate Chemical compound O=C=NC1=CC=CC=C1 DGTNSSLYPYDJGL-UHFFFAOYSA-N 0.000 description 1
- IGALFTFNPPBUDN-UHFFFAOYSA-N phenyl-[2,3,4,5-tetrakis(oxiran-2-ylmethyl)phenyl]methanediamine Chemical compound C=1C(CC2OC2)=C(CC2OC2)C(CC2OC2)=C(CC2OC2)C=1C(N)(N)C1=CC=CC=C1 IGALFTFNPPBUDN-UHFFFAOYSA-N 0.000 description 1
- ZUOUZKKEUPVFJK-UHFFFAOYSA-N phenylbenzene Natural products C1=CC=CC=C1C1=CC=CC=C1 ZUOUZKKEUPVFJK-UHFFFAOYSA-N 0.000 description 1
- 235000021317 phosphate Nutrition 0.000 description 1
- 150000003003 phosphines Chemical class 0.000 description 1
- 150000003009 phosphonic acids Chemical class 0.000 description 1
- 150000008039 phosphoramides Chemical class 0.000 description 1
- VBQCHPIMZGQLAZ-UHFFFAOYSA-N phosphorane Chemical class [PH5] VBQCHPIMZGQLAZ-UHFFFAOYSA-N 0.000 description 1
- 150000003013 phosphoric acid derivatives Chemical class 0.000 description 1
- XFZRQAZGUOTJCS-UHFFFAOYSA-N phosphoric acid;1,3,5-triazine-2,4,6-triamine Chemical compound OP(O)(O)=O.NC1=NC(N)=NC(N)=N1 XFZRQAZGUOTJCS-UHFFFAOYSA-N 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 239000000049 pigment Substances 0.000 description 1
- 238000007747 plating Methods 0.000 description 1
- 229920002493 poly(chlorotrifluoroethylene) Polymers 0.000 description 1
- 229920000058 polyacrylate Polymers 0.000 description 1
- 229920002857 polybutadiene Polymers 0.000 description 1
- 229920005668 polycarbonate resin Polymers 0.000 description 1
- 239000004431 polycarbonate resin Substances 0.000 description 1
- 239000005023 polychlorotrifluoroethylene (PCTFE) polymer Substances 0.000 description 1
- 229920000728 polyester Polymers 0.000 description 1
- 229920000573 polyethylene Polymers 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 229920001451 polypropylene glycol Polymers 0.000 description 1
- 229920002223 polystyrene Polymers 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- YOSXAXYCARLZTR-UHFFFAOYSA-N prop-2-enoyl isocyanate Chemical compound C=CC(=O)N=C=O YOSXAXYCARLZTR-UHFFFAOYSA-N 0.000 description 1
- XPGAWFIWCWKDDL-UHFFFAOYSA-N propan-1-olate;zirconium(4+) Chemical compound [Zr+4].CCC[O-].CCC[O-].CCC[O-].CCC[O-] XPGAWFIWCWKDDL-UHFFFAOYSA-N 0.000 description 1
- 125000000168 pyrrolyl group Chemical group 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 238000007650 screen-printing Methods 0.000 description 1
- 229910052624 sepiolite Inorganic materials 0.000 description 1
- 235000019355 sepiolite Nutrition 0.000 description 1
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 238000004528 spin coating Methods 0.000 description 1
- 238000005507 spraying Methods 0.000 description 1
- 238000004544 sputter deposition Methods 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- 150000003440 styrenes Chemical class 0.000 description 1
- 125000000446 sulfanediyl group Chemical group *S* 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 239000000454 talc Substances 0.000 description 1
- 229910052623 talc Inorganic materials 0.000 description 1
- 238000010345 tape casting Methods 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
- 239000012085 test solution Substances 0.000 description 1
- 238000005979 thermal decomposition reaction Methods 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 description 1
- 229910001887 tin oxide Inorganic materials 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- 238000004448 titration Methods 0.000 description 1
- RUELTTOHQODFPA-UHFFFAOYSA-N toluene 2,6-diisocyanate Chemical compound CC1=C(N=C=O)C=CC=C1N=C=O RUELTTOHQODFPA-UHFFFAOYSA-N 0.000 description 1
- QORWJWZARLRLPR-UHFFFAOYSA-H tricalcium bis(phosphate) Chemical compound [Ca+2].[Ca+2].[Ca+2].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O QORWJWZARLRLPR-UHFFFAOYSA-H 0.000 description 1
- GTOWTBKGCUDSNY-UHFFFAOYSA-K tris[[ethyl(methyl)phosphoryl]oxy]alumane Chemical compound [Al+3].CCP(C)([O-])=O.CCP(C)([O-])=O.CCP(C)([O-])=O GTOWTBKGCUDSNY-UHFFFAOYSA-K 0.000 description 1
- BIKXLKXABVUSMH-UHFFFAOYSA-N trizinc;diborate Chemical compound [Zn+2].[Zn+2].[Zn+2].[O-]B([O-])[O-].[O-]B([O-])[O-] BIKXLKXABVUSMH-UHFFFAOYSA-N 0.000 description 1
- 239000004034 viscosity adjusting agent Substances 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
- 239000010456 wollastonite Substances 0.000 description 1
- 229910052882 wollastonite Inorganic materials 0.000 description 1
- 239000011667 zinc carbonate Substances 0.000 description 1
- 229910000010 zinc carbonate Inorganic materials 0.000 description 1
- 235000004416 zinc carbonate Nutrition 0.000 description 1
- 239000011787 zinc oxide Substances 0.000 description 1
- 229910001928 zirconium oxide Inorganic materials 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
- 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
-
- 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
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
- H01B17/00—Insulators or insulating bodies characterised by their form
- H01B17/56—Insulating bodies
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
- H01B3/00—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties
- H01B3/18—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of organic substances
- H01B3/30—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of organic substances plastics; resins; waxes
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
- H01B3/00—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties
- H01B3/18—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of organic substances
- H01B3/30—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of organic substances plastics; resins; waxes
- H01B3/44—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of organic substances plastics; resins; waxes vinyl resins; acrylic resins
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
- H05K1/00—Printed circuits
- H05K1/02—Details
- H05K1/03—Use of materials for the substrate
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
- H05K1/00—Printed circuits
- H05K1/02—Details
- H05K1/03—Use of materials for the substrate
- H05K1/0313—Organic insulating material
- H05K1/0353—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement
- H05K1/0373—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement containing additives, e.g. fillers
-
- 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
- H05K3/46—Manufacturing multilayer circuits
Definitions
- the present disclosure relates to adhesive resin sheets. Furthermore, the present invention relates to a printed wiring board and an electronic device containing a cured product of the adhesive resin sheet.
- transmission loss of electrical signals is considered to consist of dielectric loss caused by the dielectric properties of insulating layers around wiring, and conductor loss caused by the shape, skin resistance, characteristic impedance, and the like of conductors.
- dielectric loss increases in proportion to the product of the square root of the dielectric constant of the material and the dielectric loss tangent of the material, both the dielectric constant and the dielectric loss tangent are Low materials are required.
- Patent Document 1 includes a first compound having a naphthylene ether skeleton and a second compound having a skeleton derived from dimer diamine or trimer triamine, and the second compound is a polyimide compound.
- a resin material is disclosed that is a different compound. It is disclosed that the resin material can reduce the dielectric loss tangent of the cured product over a wide frequency band from low to high frequencies, and that smear can be efficiently removed by desmear treatment.
- the present disclosure has been made in view of the above problems, and has an excellent dielectric loss tangent in a high frequency band, and exhibits high migration resistance even after a solder reflow process at a high temperature (for example, 280 ° C.).
- An object of the present invention is to provide an adhesive resin sheet exhibiting excellent flexibility.
- the present inventors have found that the following aspects solve the problems of the present disclosure, and have completed the present disclosure. That is, the problem is solved by providing an adhesive resin sheet characterized by satisfying i, ii, iii and iv below when heated at 180° C. for 1 hour.
- i At 23°C, the dielectric loss tangent at a measurement frequency of 10 GHz is 0.005 or less; ii: At 23°C, the dielectric loss tangent at a measurement frequency of 20 GHz is 0.007 or less; iii: At 23°C, the dielectric loss tangent at a measurement frequency of 40 GHz is 0.01 or less; iv: A mass reduction rate of 5% measured in accordance with thermogravimetry specified in JIS K7120, inflow gas: nitrogen, measurement temperature range: 25°C to 500°C, heating rate: 10°C/min. when the temperature is 280° C. or higher.
- an adhesive resin sheet that exhibits excellent dielectric loss tangent in each high frequency band of 10 GHz, 20 GHz, and 40 GHz, does not deteriorate even in a high-temperature solder reflow process, exhibits high migration resistance, and has excellent flexibility at the same time.
- an adhesive resin sheet that exhibits excellent dielectric loss tangent in each high frequency band of 10 GHz, 20 GHz, and 40 GHz, does not deteriorate even in a high-temperature solder reflow process, exhibits high migration resistance, and has excellent flexibility at the same time.
- FIG. 2 is a schematic plan view for explaining a method for producing a laminated wiring board for evaluation of migration resistance in the present disclosure
- FIG. 2 is a schematic plan view for explaining a method for producing a laminated wiring board for evaluation of migration resistance in the present disclosure
- FIG. 2 is a schematic plan view for explaining a method for producing a laminated wiring board for evaluation of migration resistance in the present disclosure
- FIG. 2 is a schematic cross-sectional view for explaining a method for producing a laminated wiring board for evaluation of migration resistance in the present disclosure
- the adhesive resin sheet of the present disclosure (hereinafter also referred to as the adhesive resin sheet) exhibits excellent dielectric loss tangent even in high frequency bands such as 10 GHz, 20 GHz, and 40 GHz when heated at 180 ° C. for 1 hour, and solder reflow. After processing, it has high migration resistance and high flexibility. Therefore, the present adhesive resin sheet is preferably used as an adhesive member for printed wiring boards and electronic devices. This adhesive resin sheet is sandwiched between members to be adhered and temporarily adhered to each other, and then heated or subjected to a hot press process to cure and adhere the adherends to each other.
- the adhesive resin sheet heated at 180° C. for 1 hour is also referred to as a cured product of the adhesive resin sheet or an adhesive layer.
- the adhesive resin sheet preferably contains a binder resin (A), a curing agent (B), a filler (C) and other optional components.
- the binder resin (A) in the present disclosure preferably functions as a substrate of the adhesive resin sheet and also has a function of maintaining the dispersed state of other components.
- the binder resin (A) in the present disclosure includes acrylic resins, polyester resins, polyurethane resins, polyurethane polyurea resins, polyamide resins, polyimide resins, polycarbonate resins, polyphenylene ether resins, styrene elastomers, fluororesins and styrene maleic anhydride resins. etc. These resins can be selected as appropriate and can be used singly or in combination.
- the binder resin (A) includes styrene-based elastomers, polyphenylene ethers, Polyimides, polyamides and polyurethanes are preferably used. From the same point of view, it is more preferable to use a styrene elastomer, polyimide, polyamide, or polyurethane as the binder resin (A).
- the styrene-based elastomer is a block copolymer in which a portion composed of styrene and a portion composed of butadiene, isoprene, ethylene, or the like form a "block".
- the binder resin (A) in the present disclosure may have a reactive functional group capable of reacting with a functional group such as an epoxy group, a maleimide group, an isocyanate group, a carbodiimide group, or a metal chelate, which the curing agent (B) may have.
- a functional group such as an epoxy group, a maleimide group, an isocyanate group, a carbodiimide group, or a metal chelate
- the curing agent (B) may have.
- the reactive functional groups include carboxyl group, acid anhydride group, hydroxyl group (alcoholic hydroxyl group, phenolic hydroxyl group), amino group, cyanate group, isocyano group, cyanato group, isocyanato group, imidazole group, pyrrole group, and acetal group.
- the reactive functional group is preferably selected from the group consisting of carboxyl group, acid anhydride group, hydroxyl group (alcoholic hydroxyl group, phenolic hydroxyl group) and amino group.
- the binder resin (A) may contain two or more reactive functional groups in its molecular structure.
- the binder resin (A) preferably has nitrogen, phosphorus and sulfur atoms.
- a binder resin (Ai) having an element having a lone pair of electrons such as nitrogen, phosphorus, and sulfur
- the interaction between the binder resin (Ai) using these lone pairs of electrons enables Since the cohesive force of the adhesive layer is improved and the movement of ions is suppressed, the migration resistance is further improved.
- the mechanism of the effects of the present disclosure is not limited to the above-described contents.
- the mass ratio of the binder resin (Ai) to the total binder resin (A) is preferably 30% by mass or more, more preferably 40% by mass or more. , more preferably 50% by mass or more.
- the mass ratio of the binder resin (Ai) to the entire binder resin (A) is set to 90% by mass or less.
- the mass ratio of the binder resin (A-ii) to the total binder resin (A) is preferably 70% by mass or less, more preferably 60% by mass or less. , 50% by mass or less.
- the mass ratio of the binder resin (A-ii) to the total binder resin (A) is set to 30% by mass or more. It is preferable to
- the acid value of the binder resin (A) is preferably 0.5-30 mgKOH/g, more preferably 1.0-20 mgKOH/g.
- the acid value is preferably 0.5-30 mgKOH/g, more preferably 1.0-20 mgKOH/g.
- the dielectric loss tangent of the binder resin (A) at 23° C. at 10 GHz, 20 GHz, and 40 GHz is preferably 0.005 or less, and 0.005 or less. 004 or less, and even more preferably 0.003 or less. It is preferable that the dielectric loss tangent of the binder resin (A) in each high frequency band is as small as possible.
- the dielectric loss tangent of the binder resin (A) is a value obtained by heating and curing only the binder resin (A) and measuring the dielectric loss tangent by the method described later.
- the water absorption of the binder resin (A) is 0.5% or less in the measurement method according to JIS K7209. Incidentally, the lower the water absorption rate of the binder resin (A), the better.
- the glass transition temperature (Tg) of the binder resin (A) is preferably 0 to 140°C, more preferably 0 to 120°C, and 0 to 100°C. is more preferred.
- the weight average molecular weight of the binder resin (A) is preferably 5,000 or more.
- the weight average molecular weight of the binder resin (A) is 5,000 or more, sufficient film formability can be easily expressed, the 5% weight decomposition temperature can be increased, and migration resistance after the solder reflow process can be improved. get better.
- the weight average molecular weight of the binder resin (A) is more preferably 20,000 or more.
- the weight average molecular weight of the binder resin (A) is preferably 200,000 or less, more preferably 150,000 or less, and 100,000 or less. It is even more preferable to have
- the curing agent (B) preferably has a functional group capable of reacting with the reactive functional group that the binder resin (A) may have, and more preferably has a plurality of such reactive functional groups.
- the curing agent (B) includes an epoxy group-containing compound (B-1), a maleimide group-containing compound (B-2), an isocyanate group-containing compound (B-3), a metal chelate compound (B-4) and a carbodiimide group-containing compound. It is preferably at least one selected from the group consisting of (B-5).
- Epoxy group-containing compound (B-1) is not particularly limited as long as it is a compound having an epoxy group in the molecule, but preferably has an average of two or more epoxy groups in one molecule. can be used.
- epoxy group-containing compound (B-1) for example, epoxy resins such as glycidyl ether-type epoxy resins, glycidylamine-type epoxy resins, glycidyl ester-type epoxy resins, and cycloaliphatic (alicyclic) epoxy resins can be used. can be done.
- Glycidyl ether type epoxy resins include, for example, bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol S type epoxy resin, bisphenol AD type epoxy resin, cresol novolak type epoxy resin, phenol novolak type epoxy resin, ⁇ -naphthol novolak. type epoxy resins, bisphenol A type novolak type epoxy resins, dicyclopentadiene type epoxy resins, tetrabromobisphenol A type epoxy resins, brominated phenol novolak type epoxy resins, tris(glycidyloxyphenyl)methane, and tetrakis(glycidyloxyphenyl) ethane and the like.
- glycidylamine-type epoxy resins examples include tetraglycidyldiaminodiphenylmethane, triglycidyl para-aminophenol, triglycidylmethaminophenol, and tetraglycidylmethaxylylenediamine.
- glycidyl ester type epoxy resins examples include diglycidyl phthalate, diglycidyl hexahydrophthalate, and diglycidyl tetrahydrophthalate.
- Cycloaliphatic (alicyclic) epoxy resins include, for example, epoxycyclohexylmethyl-epoxycyclohexanecarboxylate and bis(epoxycyclohexyl)adipate.
- epoxy group-containing compound (B-1) one of the above compounds can be used alone, or two or more of them can be used in combination.
- the epoxy group-containing compound (B-1) from the viewpoint of high adhesion, bisphenol A type epoxy resin, cresol novolak type epoxy resin, phenol novolak type epoxy resin, tris(glycidyloxyphenyl)methane, tetrakis(glycidyloxyphenyl ) ethane or tetraglycidyl-meta-xylylene diamine is preferably used.
- the epoxy group-containing compound (B-1) more preferably contains a trifunctional or higher epoxy group.
- the maleimide group-containing compound (B-2) is not particularly limited as long as it is a compound having a maleimide group in the molecule, but preferably has an average of two or more maleimide groups in one molecule. can be used.
- maleimide group-containing compound (B-2) in the present disclosure examples include o-phenylenebismaleimide, m-phenylenebismaleimide, p-phenylenebismaleimide, 4-methyl-1,3-phenylenebismaleimide, N, N'-(toluene-2,6-diyl)bismaleimide), 4,4'-diphenylmethanebismaleimide, bisphenol A diphenylether bismaleimide, 3,3'-dimethyl-5,5'-diethyl-4,4'- Diphenylmethanebismaleimide, 4,4'-diphenyletherbismaleimide, 4,4'-diphenylsulfonebismaleimide, 1,3-bis(3-maleimidophenoxy)benzene, 1,3-bis(4-maleimidophenoxy)benzene, poly Phenylmethanemaleimide (CAS NO: 67784-74-1, reaction product of polymer composed of formaldehyde
- examples of the maleimide group-containing compound (B-2) include polyfunctional maleimide obtained by reacting a polyfunctional amine with maleic anhydride.
- examples of the polyfunctional amine include isophoronediamine, dicyclohexylmethane-4,4′-diamine, and products having terminal aminated polypropylene glycol skeletons manufactured by Huntsman Corporation, trade names: Jeffamine D-230, HK-511, and D.
- the isocyanate group-containing compound (B-3) is not particularly limited as long as it is a compound having an isocyanate group in its molecule.
- Specific examples of the isocyanate group-containing compound (B-3) having one isocyanate group in one molecule include n-butyl isocyanate, isopropyl isocyanate, phenyl isocyanate, benzyl isocyanate, (meth)acryloyloxyethyl isocyanate, 1 , 1-bis[(meth)acryloyloxymethyl]ethyl isocyanate, vinyl isocyanate, allyl isocyanate, (meth)acryloyl isocyanate, isopropenyl- ⁇ , ⁇ -dimethylbenzyl isocyanate and the like.
- isocyanate group-containing compound (B-3) 1,6-diisocyanatohexane, isophorone diisocyanate, 4,4′-diphenylmethane diisocyanate, polymeric diphenylmethane diisocyanate, xylylene diisocyanate, and tolylene 2,4-diisocyanate.
- isocyanate group-containing compound (B-3) having two isocyanate groups in one molecule include 1,3-phenylene diisocyanate, 4,4′-diphenyl diisocyanate, 1,4-phenylene diisocyanate, 4 ,4'-diphenylmethane diisocyanate, 2,4-tolylene diisocyanate, 2,6-tolylene diisocyanate, 4,4'-toluidine diisocyanate, 2,4,6-triisocyanatotoluene, 1,3,5-triisocyanatobenzene , dianisidine diisocyanate, 4,4′-diphenyl ether diisocyanate, 4,4′,4′′-triphenylmethane triisocyanate and other aromatic diisocyanates, trimethylene diisocyanate, tetramethylene diisocyanate, hexamethylene diisocyanate, pentamethylene diisocyanate, 1,2-propylene diisocyan
- isocyanate group-containing compound (B-3) having three isocyanate groups in one molecule specifically, aromatic polyisocyanate, aliphatic polyisocyanate such as lysine triisocyanate, araliphatic polyisocyanate, alicyclic polyisocyanate and the like. Further, specific examples thereof include the above-described trimethylolpropane adduct of diisocyanate, water-reacted biuret form, and trimer having an isocyanurate ring.
- isocyanate group-containing compound (B-3) a blocked isocyanate group-containing compound in which the isocyanate group in the various illustrated isocyanate group-containing compounds is protected with ⁇ -caprolactam, MEK oxime, or the like can also be used. Specific examples include those obtained by blocking the isocyanate group of the isocyanate group-containing compound with ⁇ -caprolactam, methyl ethyl ketone (hereinafter also referred to as MEK) oxime, cyclohexanone oxime, pyrazole, phenol, and the like.
- MEK methyl ethyl ketone
- the isocyanate group-containing compound (B-3) preferably has a trifunctional or higher isocyanate group.
- the metal chelate compound (B-4) is an organometallic compound composed of a metal and an organic substance, and reacts with the reactive functional groups of the binder resin (A) to form crosslinks.
- organometallic compound is not particularly limited, examples thereof include organoaluminum compounds, organotitanium compounds, and organozirconium compounds.
- the bond between the metal and the organic substance may be a metal-oxygen bond, and is not limited to a metal-carbon bond.
- the bonding mode between the metal and the organic substance may be any of chemical bond, coordinate bond, and ionic bond.
- the organometallic compound is preferably trifunctional or higher from the viewpoint of heat resistance.
- the organoaluminum compound is preferably an aluminum metal chelate compound.
- aluminum metal chelate compounds include ethylacetoacetate aluminum diisopropylate, aluminum tris(ethylacetoacetate), alkylacetoacetate aluminum diisopropylate, aluminum monoacetylacetonate bis(ethylacetoacetate), aluminum tris(acetylacetate ), aluminum monoacetylacetate bis(ethylacetoacetate), aluminum di-n-butoxide monomethylacetoacetate, aluminum diisobutoxide monomethylacetoacetate, aluminum di-sec-butoxide monomethylacetoacetate, aluminum isopropylate, monosec-butoxy aluminum diisopropylate, aluminum-sec-butyrate, aluminum ethylate and the like.
- the organic titanium compound is preferably a titanium metal chelate compound.
- titanium metal chelate compounds include titanium acetylacetonate, titanium tetraacetylacetonate, titanium ethylacetoacetate, titanium octylene glycolate, titanium ethylacetoacetate, titanium-1,3-propanedioxybis(ethylacetoacetate).
- polytitanium acetyl acetylacetonate polytitanium acetyl acetylacetonate, tetraisopropyl titanate, tetra-n-butyl titanate, butyl titanate dimer, tetraoctyl titanate, d'amyl titanate, tetra-tert-butyl titanate, tetrastearyl titanate, titanium isostearate, tri-n- butoxytitanium monostearate, di-i-propoxytitanium distearate, titanium stearate, di-i-propoxytitanium diisostearate, (2-n-butoxycarbonylbenzoyloxy)tributoxytitanium and the like.
- the organic zirconium compound is preferably a zirconium metal chelate compound.
- zirconium metal chelate compounds include zirconium tetraacetylacetonate, zirconium tributoxyacetylacetonate, zirconium monobutoxyacetylacetonate bis(ethylacetoacetate), zirconium dibutoxybis(ethylacetoacetate), and zirconium tetraacetylacetonate. , normal propyl zirconate, normal butyl zirconate, zirconium stearate, zirconium octylate and the like.
- the metal chelate compound (B-4) is preferably an organic titanium compound or an organic zirconium compound from the viewpoint of thermosetting reactivity.
- Carbodiimide group-containing compound (B-5) The carbodiimide group-containing compound (B-5) is not particularly limited as long as it has a carbodiimide group in its molecule.
- Carbodiimide group-containing compounds (B-5) include, for example, Carbodilite V-01, V-03, V-05, V-07, V-09 (trade name, Nisshinbo Chemical Co., Ltd.), cyclic carbodiimide (Teijin Limited ) and the like. From the viewpoint of heat resistance, the carbodiimide group-containing compound (B-5) preferably has an average of 3 or more carbodiimide groups per molecule.
- the content of the curing agent (B) is preferably 1 to 30 parts by mass in total with respect to 100 parts of the binder resin (A).
- the amount of the curing agent (B) added to the present adhesive resin sheet is 1 to 30 parts by mass, the content of polar groups derived from the curing agent (B) contained in the present adhesive resin sheet can be reduced. , it becomes easier to keep the dielectric loss tangent lower.
- the amount of the curing agent (B) added in this way it becomes easier to control the glass transition temperature (Tg) of the adhesive layer in a preferable range, and it is easy to achieve both high flexibility and low dielectric loss tangent. can be realized.
- the content of the curing agent (B) with respect to 100 parts of the binder resin (A) in the present adhesive resin sheet is more preferably 1 to 20 parts by mass, more preferably 1 to 10 parts by mass. It is even more preferable to have
- the functional group equivalent weight of the curing agent (B) is preferably 50-1,000 g/eq, more preferably 50-500 g/eq, still more preferably 50-300 g/eq.
- the functional group equivalent weight of the curing agent (B) is preferably 50-1,000 g/eq, more preferably 50-500 g/eq, still more preferably 50-300 g/eq.
- the curing agent (B) preferably has an aromatic structure in its structure.
- This adhesive resin sheet preferably contains a filler (C) from the viewpoint of increasing the 5% weight decomposition temperature and improving the migration resistance after the solder reflow process.
- the filler (C) is not particularly limited, but may be spherical, powdery, fibrous, needle-like, scale-like, or the like.
- Examples of the filler (C) include polytetrafluoroethylene powder and modified products thereof, tetrafluoroethylene-perfluoroalkylvinyl ether powder, tetrafluoroethylene-ethylene powder, tetrafluoroethylene-hexafluoropropylene powder, tetrafluoroethylene-fluoride.
- Vinylidene chloride powder tetrafluoroethylene-hexafluoropropylene-perfluoroalkyl vinyl ether powder, polychlorotrifluoroethylene powder, chlorotrifluoroethylene-ethylene powder, chlorotrifluoroethylene-vinylidene fluoride powder, polyvinylidene fluoride powder, polyvinylidene fluoride fluorine-based fillers such as vinyl powder; Polyethylene powder, polyacrylate powder, epoxy resin powder, polyamide powder, polyimide powder, polyurethane powder, liquid crystal polymer, polysiloxane powder, etc., as well as multi-layered core shells using silicone, acrylic, styrene-butadiene rubber, butadiene rubber, etc.
- polymeric fillers such as; (Poly)phosphates such as melamine phosphate, melamine polyphosphate, guanidine phosphate, guanidine polyphosphate, ammonium phosphate, ammonium polyphosphate, amide ammonium phosphate, amide ammonium polyphosphate, carbamate phosphate, and carbamate polyphosphate phosphines such as compounds, organophosphate compounds, phosphazene compounds, phosphonic acid compounds, aluminum diethylphosphinate, aluminum methylethylphosphinate, aluminum diphenylphosphinate, aluminum ethylbutylphosphinate, aluminum methylbutylphosphinate, and aluminum polyethylenephosphinate
- Phosphorus-based fillers such as acid compounds, phosphine oxide compounds, phosphorane compounds, and phosphoramide compounds; Nitrogen-based fillers such as benzoguanamine, melamine, melam, melem, melon, mel
- the filler (C) is at least one selected from fluorine-based fillers, boron nitride, liquid crystal polymers, silica and phosphorus-based fillers. is preferred. From the same point of view, it is more preferable to use at least one selected from fluorine-based fillers, boron nitride, phosphorus-based fillers, and silica as the filler (C). Since these fillers have a strong crystal structure, they have small molecular vibrations and excellent dielectric loss tangent even in a high frequency band. In the present disclosure, the filler (C) can be used alone or in combination. In the present disclosure, liquid crystal polymer refers to a granular substance.
- the content of the filler (C) in the adhesive resin sheet is preferably 3 to 50% by mass, more preferably 4 to 30% by mass, based on the total mass of the adhesive resin sheet. 8 to 25 mass % is particularly preferred.
- the content of the filler (C) in the present adhesive resin sheet is preferably 3 to 50% by mass, more preferably 4 to 30% by mass, based on the total mass of the adhesive resin sheet. 8 to 25 mass % is particularly preferred.
- the content of the filler (C) is more preferably 4% by mass or more, particularly preferably 8% by mass or more.
- the content of the filler (C) is more preferably 30% by mass or less, and particularly preferably 25% by mass or less.
- the filler (C) preferably has a dielectric loss tangent at 10 GHz at 23° C. of 0.005 or less, more preferably 0.004 or less, and preferably 0.003 or less. More preferred.
- the dielectric loss tangent of the filler (C) is preferably as small as possible.
- the average particle size D 50 of the filler (C) is preferably 0.1 to 25 ⁇ m.
- the average particle diameter D50 of the filler (C) is from 0.1 to 25 ⁇ m, improvement in coatability can be expected.
- the average particle diameter D50 of the filler (C) is more preferably 1.0 to 10 ⁇ m.
- the method of adding the filler (C) is not particularly limited, and any conventionally known method may be used. Specifically, this addition method includes a method of adding the filler (C) to the polymerization reaction solution before or during the polymerization of the binder resin (A), and a method of adding the filler (C) to the binder resin (A) using a three-roll roll or the like. Examples include a method of kneading the filler (C), a method of preparing a dispersion containing the filler (C), and mixing this dispersion with the binder resin (A). Further, in order to disperse the filler (C) satisfactorily and stabilize the dispersed state, dispersants, thickeners, etc. may be used as long as they do not affect the physical properties of the adhesive resin sheet.
- the present adhesive resin sheet may further contain energy ray absorbers, dyes, pigments, antioxidants, polymerization inhibitors, antifoaming agents, leveling agents, and ion traps as optional components within a range that does not impair the purpose.
- a collector, a humectant, a viscosity modifier, an antiseptic, an antibacterial agent, an antistatic agent, an antiblocking agent, an infrared absorber, an electromagnetic wave shielding agent, and the like can be added.
- the cured product of the adhesive resin sheet in the present disclosure has (i) a dielectric loss tangent of 0.005 or less at a measurement frequency of 10 GHz and (ii) a dielectric loss tangent of 0.007 or less at a measurement frequency of 20 GHz at 23 ° C. and (iii) the dielectric loss tangent at a measurement frequency of 40 GHz is 0.01 or less.
- the dielectric loss tangent is within the above numerical range, the transmission loss of electrical signals in the electronic device is improved.
- the cured product (adhesive layer) of the adhesive resin sheet in the present disclosure applied to the electronic device satisfies the above-described (i), (ii), and (iii), which means that the adjacent circuit This is very effective in improving the transmission loss of electrical signals.
- the dielectric loss tangent of the adhesive layer is 0.005 or less, preferably 0.004 or less at 23° C. and a measurement frequency of 10 GHz, preferably 0.003. It is more preferably 0.002 or less, particularly preferably 0.002 or less. Further, from the viewpoint of transmission loss of electrical signals, the dielectric loss tangent of the adhesive layer is 0.007 or less, preferably 0.006 or less, and preferably 0.005 or less at 23° C. and a measurement frequency of 20 GHz. It is more preferably 0.004 or less, particularly preferably 0.004 or less.
- the dielectric loss tangent of the adhesive layer is 0.010 or less, preferably 0.008 or less, and preferably 0.007 or less at 23° C. and a measurement frequency of 40 GHz. It is more preferably 0.006 or less, and particularly preferably 0.006 or less. The smaller the dielectric loss tangent of the adhesive layer at each measurement frequency, the better.
- the dielectric loss tangent of the adhesive layer (hereinafter also referred to as the adhesive layer) in the present disclosure can be controlled by the type of binder resin (A).
- the binder resin (A) is preferably a styrene-based elastomer, polyimide, polyamide or polyurethane.
- the adhesive layer satisfying the specific dielectric loss tangent in the present disclosure includes the content and functional group equivalent of the curing agent (B), the content of the filler (C), the filler ( It can be realized by controlling the dielectric loss tangent of C).
- the thermal stability of this adhesive layer can be determined by a measurement method conforming to the thermogravimetry method specified in JIS K7120.
- the adhesive layer obtained by heating the adhesive resin sheet at 180° C. for 1 hour satisfies the following condition (iv). That is, (iv) in accordance with the thermogravimetric measurement specified in JISK 7120, inflow gas: nitrogen, measurement temperature range: 25 ° C. to 500 ° C., heating rate: 10 ° C./min, the mass reduction rate measured is 5. % (hereinafter also referred to as 5% weight decomposition temperature) is 280° C. or higher.
- the 5% weight decomposition temperature is defined as the temperature at which the weight of the adhesive layer is reduced by 5% due to the temperature rise when the weight of the adhesive layer before measurement is 100%. Since the 5% weight decomposition temperature of the present adhesive layer is 280 ° C. or higher, there are application examples of the present adhesive resin sheet and solder reflow, which is one of electronic component mounting processes for printed wiring boards, which is another aspect of the present disclosure. Volatile components (outgassing) in the process can be reduced. In addition, phenomena such as delamination and foaming (blistering) due to thermal expansion of outgas can be suppressed, and migration resistance after the solder reflow process is improved.
- the 5% weight decomposition temperature of the present adhesive layer is preferably 290° C. or higher, more preferably 300° C. or higher.
- the 5% weight decomposition temperature of the adhesive layer is preferably 500° C. or lower, more preferably 450° C. or lower, from the viewpoint of efficiency of incineration in waste treatment of printed wiring boards.
- the 5% weight decomposition temperature of this adhesive layer can be determined by controlling the amount of filler (C) added, changing the type of binder resin (A), using a binder resin (A) having a specific molecular weight, using a specific structure (fragrance It can be controlled by using a curing agent (B) having a group structure), adjusting the functional group equivalent of the curing agent (B), and the like.
- the glass transition temperature (Tg) of the cured product (adhesive layer) of the present adhesive resin sheet is preferably 0 to 150°C.
- Tg of the adhesive layer is 0° C. or higher, the dielectric loss tangent of the adhesive layer can be further reduced.
- the Tg of the present adhesive layer is more preferably 40°C or higher, and even more preferably 70°C or higher. If the Tg of the adhesive layer is 150° C. or less, the flexibility of the adhesive layer can be improved. From the same point of view, the Tg of the present adhesive layer is more preferably 120° C. or lower, and even more preferably 100° C. or lower.
- the Tg of the adhesive layer can be measured using a DVA (dynamic viscoelasticity analysis) measuring device or the like. From the viscoelastic curve of the adhesive layer obtained by the apparatus, the ratio of storage modulus/loss modulus (tan ⁇ ) at each temperature can be obtained. It can be determined as the Tg of the layer. When there are a plurality of maximum points in the tan ⁇ curve, the highest maximum point is taken as the Tg of the adhesive layer.
- the Tg of this adhesive layer can be controlled by the glass transition temperature of the binder resin (A) and the amount of the curing agent (B).
- the method for producing the present adhesive resin sheet is not particularly limited, but for example, the following method can be adopted. First, a coating solution containing a binder resin (A), a curing agent (B), a filler (C), other optional components, and a solvent is applied to one side of a release film. Subsequently, a liquid medium such as an organic solvent contained in the coating solution is removed and dried, usually at 40 to 150° C., to form an adhesive resin sheet. An adhesive resin sheet with a double-sided release film may be produced by laminating another release film on the surface of the obtained adhesive resin sheet. By laminating the release films on both sides of the adhesive resin sheet, surface contamination of the adhesive resin sheet can be prevented.
- a coating solution containing a binder resin (A), a curing agent (B), a filler (C), other optional components, and a solvent is applied to one side of a release film.
- a liquid medium such as an organic solvent contained in the coating solution is removed and dried, usually at 40 to 150° C.
- the adhesive resin sheet can be isolated by peeling off the release film.
- the two release films can be of the same type or of different types.
- release films with different release properties on both sides of the adhesive resin sheet it is possible to vary the strength of the release force, making it easier to peel off in order during use.
- Examples of methods for applying the coating solution include comma coating, knife coating, die coating, lip coating, roll coating, curtain coating, bar coating, gravure printing, flexographic printing, screen printing, dip coating, spray coating, spin coating, and the like. , a known method can be selected.
- the thickness of the adhesive resin sheet after drying is preferably 5 ⁇ m to 500 ⁇ m, more preferably 10 ⁇ m to 100 ⁇ m, from the viewpoints of sufficient adhesion and ease of handling.
- a copper-clad laminate or a printed wiring board can be obtained using the present adhesive resin sheet or the like.
- the present adhesive resin sheet can be used for copper-clad laminates and printed wiring boards. Also, these will be described in detail below.
- a copper-clad laminate is obtained by laminating a copper foil and an insulating film via an adhesive layer, which is a cured product of the present adhesive resin sheet.
- Such a copper-clad laminate can be obtained, for example, by the following method. That is, the peelable films are sequentially peeled off from the adhesive resin sheet with the peelable film, and the copper foil and the insulating film are overlaid on each surface of the adhesive resin sheet (this step is also called temporary adhesion). Subsequently, the obtained laminate is subjected to a heating or hot pressing step to thermally cure the adhesive resin sheet between the copper foil and the insulating film, thereby obtaining the copper-clad laminate.
- a copper-clad laminate can be obtained by the following method.
- a coating solution for forming an adhesive resin sheet is applied and dried on an insulating film, a copper foil is placed on the formed adhesive resin sheet, and the copper foil and insulating properties are obtained by heating or a hot press process.
- a copper-clad laminate can also be obtained by thermosetting the adhesive resin sheet between the film.
- the copper-clad laminate may have both outermost layers of copper foil, such as copper foil/adhesive layer/insulating film/adhesive layer/copper foil, or may be provided with an inner layer of copper foil. .
- the plurality of adhesive resin sheets can be heat-cured at once after temporary adhesion has been performed a plurality of times.
- the printed wiring board (hereinafter also referred to as the printed wiring board) in the present disclosure includes the cured product of the adhesive resin sheet.
- the present printed wiring board can be obtained by processing the copper foil in the copper-clad laminate described above by etching or the like to form a signal circuit and a ground circuit.
- the signal circuit can be protected or used as a substrate for further multilayering.
- a photosensitive etching resist layer is formed on the copper foil of the copper-clad laminate, exposed through a mask film having a circuit pattern, and only the exposed portions are cured. Then, after removing the unexposed portions of the copper foil by etching, a conductive circuit can be formed from the copper foil by, for example, peeling off the remaining resist layer.
- this printed wiring board can also be produced without using the copper-clad laminate described above.
- a conductive pattern is formed on a flexible and insulating plastic film such as polyester, polyimide, liquid crystal polymer, or PTFE film by printing technology.
- a protective layer is laminated via the present adhesive resin sheet so as to cover the conductor pattern, and the adhesive resin sheet is cured by heating and pressing to obtain a flexible printed wiring board provided with a protective layer.
- a flexible print in which only necessary circuits are provided on a flexible and insulating plastic film by means of sputtering, plating, etc., and a protective layer is provided via the cured product of this adhesive resin sheet in the same way thereafter.
- a wiring board can also be obtained.
- the present adhesive resin sheet is sandwiched between a plurality of flexible printed wirings, and the adhesive resin sheet is cured by applying heat and pressure to use the present adhesive resin sheet as an interlayer bonding resin sheet. be able to.
- a multilayer flexible printed wiring board or the like can be obtained.
- This printed wiring board has via openings such as blind vias and through-holes in order to conduct conduction between adhesive layers obtained by curing this adhesive resin sheet and multiple copper foils sandwiching a protective layer.
- via openings such as blind vias and through-holes in order to conduct conduction between adhesive layers obtained by curing this adhesive resin sheet and multiple copper foils sandwiching a protective layer.
- a via opening is usually formed by laser processing using a laser beam or drilling using a drill. Among these, it is preferable to form the via opening by laser processing from the viewpoint of improving the shape accuracy of the via opening.
- an electronic device such as smartphones, tablet terminals, and cameras can be manufactured using this printed wiring board. That is, an electronic device according to the present disclosure includes the printed wiring board.
- Acid value (mgKOH/g) (5.611 x a x F)/S S: Sample collection amount (g) a: consumption of 0.1N alcoholic potassium hydroxide solution (ml) F: Titer of 0.1N alcoholic potassium hydroxide solution
- the average particle diameter D50 of the filler (C) is a numerical value obtained by measuring with a Tornado dry powder sample module using a laser diffraction/scattering particle size distribution analyzer, trade name: LS13320 (manufactured by Beckman Coulter). is the particle diameter at which the cumulative value in the particle diameter cumulative distribution is 50%.
- the refractive index was set to 1.6.
- Binder resin (A)>> (A-1): Styrene-based elastomer, trade name: FG1901GT (maleic acid-modified styrene-based elastomer), acid value 10 mgKOH/g, weight average molecular weight 95,000, Tg 80°C (manufactured by Kraton). (A-2): Polyimide resin, acid value 9 mgKOH/g, weight average molecular weight 45,000, Tg 50° C.
- C-1 Trade name: SC2050-MB (silica, average particle size D 50 : 0.5 ⁇ m), manufactured by Admatechs (C-2): Trade name: SP-2 (boron nitride, average particle size D 50 ; 4.0 ⁇ m), manufactured by Denka (C-3): trade name: KT-300 (fluorine-based filler, average particle size D 50 : 10.0 ⁇ m), manufactured by Kitamura (C-4): trade name: E101-S (liquid crystal polymer, average particle size D 50 : 17.5 ⁇ m), manufactured by Sumitomo Chemical Co., Ltd.
- C-5 trade name: Exolit OP935 (aluminum phosphinate, average particle size D 50 : 2.5 ⁇ m) ), manufactured by Clariant (C-6): trade name: HT grade (alumina, average particle diameter D 50 ; 1.2 ⁇ m), manufactured by Tokuyama
- Example 1 ⁇ Manufacturing of coating liquid>>
- 100 parts of the binder resin (A-1), 5 parts of the curing agent (B-1), and 10 parts of the filler (C-1) are charged into a container so that the nonvolatile content concentration becomes 30%.
- the obtained coating solution is applied to a heavy release film (polyethylene terephthalate (PET) film coated with a heavy release agent) having a thickness of 50 ⁇ m using a doctor blade so that the thickness after drying becomes 25 ⁇ m. It was uniformly coated and dried at 100° C. for 2 minutes. Then, it was cooled to room temperature (for example, 25° C.) to obtain an adhesive resin sheet with a single-sided release film. Next, the adhesive resin sheet surface of the obtained adhesive resin sheet with a single-sided release film was superposed on a 50 ⁇ m-thick light release film (polyethylene terephthalate (PET) film coated with a light release agent).
- PET polyethylene terephthalate
- the vacuum lamination conditions were a heating temperature of 90° C., a vacuum time of 60 seconds, a vacuum ultimate pressure of 2 hPa, a pressure of 0.4 MPa, and a pressing time of 60 seconds.
- the adhesive resin sheet with the double-sided release film was pressed at 180° C. and 2 MPa for 1 hour, the release film was peeled off, and the cured product of the adhesive resin sheet was used as a test piece for measurement.
- a dielectric loss tangent was obtained at a frequency of 10 GHz.
- Similar test pieces were measured using resonators of corresponding frequencies.
- ⁇ Glass transition temperature (Tg)> (Preparation of adhesive layer for measurement) Using a doctor blade, the coating liquid used in each example and each comparative example was applied to a 50 ⁇ m thick heavy release film (polyethylene terephthalate coated with a heavy release agent) so that the thickness after drying was 200 ⁇ m. (PET) film) and dried at 100° C. for 2 minutes. Then, it was cooled to room temperature (for example, 25° C.) to form an adhesive resin sheet with a single-sided release film.
- PET polyethylene terephthalate coated with a heavy release agent
- the adhesive resin sheet surface of the obtained adhesive resin sheet with a single-sided release film is superimposed on a 50 ⁇ m-thick light release film (polyethylene terephthalate (PET) film coated with a light release agent) to form a heavy release film.
- An adhesive resin sheet with a double-sided release film consisting of /adhesive resin sheet/light release film was obtained.
- the obtained adhesive resin sheet with a double-sided release film was heat-cured at 180° C. for 1 hour at 2 MPa, and the heavy release film and the light release film were separated to obtain an adhesive layer of 200 ⁇ m.
- Tg glass transition temperature
- FIGS. 1A to 1D A method for evaluating migration resistance will be described with reference to FIGS. 1A to 1D.
- a laminate of a copper foil with a thickness of 12 ⁇ m and a polyimide film with a thickness of 25 ⁇ m was etched.
- a cathode electrode comb-shaped signal wiring 2 having a cathode electrode connection point 2p of line/space 0.05 mm/0.05 mm
- An anode electrode comb-shaped signal wiring 3 having an anode electrode connection point 3p was formed.
- FIG. 1D A method for evaluating migration resistance will be described with reference to FIGS. 1A to 1D.
- the cathode electrode comb-shaped signal wiring 2 and the anode electrode comb-shaped signal wiring 3 shown in FIG. 1A are covered, and near the cathode electrode connection point 2p and the vicinity of the anode electrode connection point 3p
- An adhesive resin sheet with a double-sided release film was pasted to the extent that the was exposed. Specifically, the surface of the adhesive resin sheet with the double-sided release film from which the light release film was removed was attached to the above-described portion and temporarily adhered with a vacuum laminator. Thereafter, the heavy release film of the adhesive resin sheet was peeled off, and a copper clad laminate 5 (CCL) composed of copper foil 5a and insulating layer 5b was adhered thereon.
- CCL copper clad laminate 5
- the insulating layer 5b of the copper-clad laminate 5 is temporarily adhered with a vacuum laminator so as to be in contact with the adhesive resin sheet before curing, and then heated at 180° C. for 1 hour at 2 MPa with a hot press. It was cured to obtain a laminated wiring board A for evaluation in which a single-sided CCL was arranged on the adhesive layer (cured product 4 of the adhesive resin sheet).
- FIG. 1C shows a schematic plan view of the produced laminated wiring board for evaluation
- FIG. 1D shows a schematic cross-sectional view of the laminated wiring board for evaluation of FIG. 1C cut along the line ID-ID.
- laminate wiring board A for evaluation was subjected to a solder float treatment.
- Laminated wiring board A for evaluation was floated on molten solder at 288° C. for 10 seconds with the polyimide film 1 side down, and a sample (laminated wiring board A for evaluation) was taken out.
- B The resistance value after 1000 hours is 1.0 ⁇ 10 8 ⁇ or more and the number of leak touches is 1, or the resistance value after 1000 hours is 1.0 ⁇ 10 8 ⁇ or more. The resistance is less than 0 ⁇ 10 10 ⁇ and the number of leak touches is 0.
- C The resistance value after 1000 hours is 1.0 ⁇ 10 7 ⁇ or more and the number of leak touches is 2, or the resistance value after 1000 hours is 1.0 ⁇ 10 7 ⁇ or more. Less than 0 ⁇ 10 8 ⁇ and the number of leak touches is 1 or less.
- D The resistance value after 1000 hours is less than 1.0 ⁇ 10 7 ⁇ , or the number of leak touches is 3 or more.
- the 5% weight decomposition temperature was measured using TGDTA220 (trade name) (manufactured by Seiko Instruments Inc.) for the cured product (adhesive layer) of the adhesive resin sheet prepared in the same manner as the dielectric loss tangent measurement. .
- Weight change (%) weight at each temperature (g) / weight of cured product before measurement (g) x 100
- the obtained 5% weight decomposition temperature was evaluated based on the following evaluation criteria to evaluate the heat resistance of the adhesive layer.
- Examples 2 to 25, Comparative Examples 1 to 2 As shown in Tables 1 to 3, an adhesive resin sheet was obtained in the same manner as in Example 1, except that the types and amounts of the binder resin (A), curing agent (B), and filler (C) were changed. , was similarly evaluated.
- the cured product of this adhesive resin sheet can achieve a lower dielectric loss tangent in high frequency bands (10 GHz, 20 GHz, 40 GHz), and can exhibit high migration resistance and excellent flexibility after the solder reflow process. Therefore, the present adhesive resin sheet can be suitably used for manufacturing printed wiring boards, electronic devices, and the like, which require high reliability and flexibility.
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Abstract
Description
一般に、電気信号の伝送損失は、配線周辺の絶縁層の誘電特性等に起因する誘電体損失と、導体の形状、表皮抵抗、特性インピーダンス等に起因する導体損失とからなるとされている。しかし、高周波回路の場合は誘電体損失の影響が大きく、誘電体損失が材料の比誘電率の平方根と材料の誘電正接の積に比例して大きくなるため、比誘電率と誘電正接がいずれも低い材料が求められている。中でも、誘電正接は誘電体損失と比例関係にあり、比誘電率よりも誘電体損失に与える影響が大きいといった理由から誘電正接を低くすることが重要であった。
例えば、下記の特許文献1には、ナフチレンエーテル骨格を有する第1の化合物と、ダイマージアミンまたはトリマートリアミンに由来する骨格を有する第2の化合物とを含み、第2の化合物がポリイミド化合物とは異なる化合物である、樹脂材料が開示されている。そして、当該樹脂材料により、低周波数帯から高周波数帯の広い周波数帯に亘って、硬化物の誘電正接を低くでき、かつデスミア処理によってスミアを効率的に除去できることが開示されている。
更に、電子デバイスの小型化、高性能化に伴い、プリント配線板における回路の細線化、ライン(配線幅)/スペース(配線間隔)への信頼性要求が厳しくなっている。そのため、回路間に用いられる接着性樹脂シートの硬化物は、高いマイグレーション耐性も必要とされている。
一方、環境保護を背景とした鉛フリーはんだへの切り替えによって、プリント配線板に電子部品を実装するはんだリフロー工程が高温化している。リフロー工程の熱で接着性樹脂シートの硬化物が劣化しマイグレーション耐性が著しく低下する場合があった。
i: 23℃において、測定周波数10GHzでの誘電正接が0.005以下である;
ii: 23℃において、測定周波数20GHzでの誘電正接が0.007以下である;
iii: 23℃において、測定周波数40GHzでの誘電正接が0.01以下である;
iv: JIS K7120に規定された熱重量測定に準拠し、流入ガス:窒素、測定温度範囲:25℃~500℃、加熱速度:10℃/分、にて測定した質量減少率が5%であるときの温度が280℃以上である。
本開示の接着性樹脂シート(以降、本接着性樹脂シートとも称する)は180℃で1時間加熱した際に、10GHz、20GHz、40GHzといった各高周波数帯でも優れた誘電正接を発現し、はんだリフロー工程後に、高いマイグレーション耐性、高屈曲性を有する。このため、本接着性樹脂シートは、プリント配線板、および電子機器の接着用部材に用いることが好ましい。本接着性樹脂シートは接着したい部材同士の間に挟み仮接着を行った後に加熱、もしくは熱プレス工程を経ることにより硬化し、被着体同士を接着する。なお、以降、180℃で1時間加熱した接着性樹脂シートを、接着性樹脂シートの硬化物又は接着剤層とも称する。
本開示におけるバインダー樹脂(A)は、接着性樹脂シートの基体として機能する他、他成分の分散状態を保持する機能を有することが好ましい。
なお、上記スチレン系エラストマーとは、スチレンから構成される部分と、ブタジエンやイソプレンやエチレン等から構成される部分とが、「ブロック」を成している、ブロック共重合体をいう。
前記反応性官能基としては、カルボキシル基、酸無水物基、水酸基(アルコール性水酸基、フェノール性水酸基)、アミノ基、シアネート基、イソシアノ基、シアナト基、イソシアナト基、イミダゾール基、ピロール基、アセタール基、アクリロイル基、メタクリロイル基、ビニル基、アルデヒド基、ヒドラジド基、ヒドラゾン基、リン酸基等が挙げられる。この中でも、前記反応性官能基は、カルボキシル基、酸無水物基、水酸基(アルコール性水酸基、フェノール性水酸基)、およびアミノ基からなる群より選ばれることが好ましい。バインダー樹脂(A)は、分子構造中に2種類以上の反応性官能基を含んでもよい。
すなわち、マイグレーション耐性向上の観点から、バインダー樹脂(A)全体に占める、バインダー樹脂(A-i)の質量割合を、30質量%以上とすることが好ましく、40質量%以上とすることがより好ましく、50質量%以上とすることが更に好ましい。また、凝集力を過度に高めず、被着体への表面密着力を向上させる観点から、バインダー樹脂(A)全体に占める、バインダー樹脂(A-i)の質量割合を、90質量%以下とすることが好ましく、80質量%以下とすることがより好ましく、70質量%以下とすることが更に好ましい。
また、マイグレーション耐性向上の観点から、バインダー樹脂(A)全体に占める、バインダー樹脂(A-ii)の質量割合を、70質量%以下とすることが好ましく、60質量%以下とすることがより好ましく、50質量%以下とすることが更に好ましい。さらに、極性の高い官能基の濃度を低下させ、接着性樹脂シートの吸水を抑制する観点から、バインダー樹脂(A)全体に占める、バインダー樹脂(A-ii)の質量割合を、30質量%以上とすることが好ましい。
硬化剤(B)は、バインダー樹脂(A)が有し得る反応性官能基と反応可能な官能基を有することが好ましく、この反応可能な官能基を複数有することがより好ましい。
硬化剤(B)は、エポキシ基含有化合物(B-1)、マレイミド基含有化合物(B-2)、イソシアネート基含有化合物(B-3)、金属キレート化合物(B-4)およびカルボジイミド基含有化合物(B-5)からなる群より選ばれる少なくとも1種であることが好ましい。これらの硬化剤を用いることで、接着剤層の耐熱性を一層上げることができ、はんだリフロー工程後のマイグレーション耐性が一層向上する。硬化剤は、単独で、または2種以上を組み合わせて用いることができる。
エポキシ基含有化合物(B-1)としては、エポキシ基を分子内に有する化合物であればよく、特に限定されるものではないが、1分子中に平均2個以上のエポキシ基を有するものを好ましく用いることができる。エポキシ基含有化合物(B-1)としては、例えば、グリジシルエーテル型エポキシ樹脂、グリジシルアミン型エポキシ樹脂、グリシジルエステル型エポキシ樹脂、および環状脂肪族(脂環型)エポキシ樹脂などのエポキシ樹脂を用いることができる。
エポキシ基含有化合物(B-1)としては、高接着性の観点から、ビスフェノールA型エポキシ樹脂、クレゾールノボラック型エポキシ樹脂、フェノールノボラック型エポキシ樹脂、トリス(グリシジルオキシフェニル)メタン、テトラキス(グリシジルオキシフェニル)エタン、又はテトラグリシジルメタキシリレンジアミンを用いることが好ましい。また、耐熱性の観点から、エポキシ基含有化合物(B-1)は、3官能以上のエポキシ基を含有しているものがより好ましい。
マレイミド基含有化合物(B-2)としては、マレイミド基を分子内に有する化合物であればよく、特に限定されるものではないが、1分子中に平均2個以上のマレイミド基を有するものを好ましく用いることができる。
イソシアネート基含有化合物(B-3)としては、イソシアネート基を分子内に有する化合物であればよく、特に限定されるものではない。
1分子中にイソシアネート基を1個有するイソシアネート基含有化合物(B-3)としては、具体的には、n-ブチルイソシアネート、イソプロピルイソシアネート、フェニルイソシアネート、ベンジルイソシアネート、(メタ)アクリロイルオキシエチルイソシアネート、1,1-ビス[(メタ)アクリロイルオキシメチル]エチルイソシアネート、ビニルイソシアネート、アリルイソシアネート、(メタ)アクリロイルイソシアネート、イソプロペニル-α,α-ジメチルベンジルイソシアネート等が挙げられる。
また、イソシアネート基含有化合物(B-3)として、1,6-ジイソシアナトヘキサン、ジイソシアン酸イソホロン、ジイソシアン酸4,4’-ジフェニルメタン、ポリメリックジフェニルメタンジイソシアネート、キシリレンジイソシアネート、2,4-ジイソシアン酸トリレン、ジイソシアン酸トルエン、2,4-ジイソシアン酸トルエン、ジイソシアン酸ヘキサメチレン、ジイソシアン酸4-メチル-m-フェニレン、ナフチレンジイソシアネート、パラフェニレンジイソシアネート、テトラメチルキシリレンジイソシアネート、シクロヘキシルメタンジイソシアネート、水添キシリレンジイソシアネート、シクロヘキシルジイソシアネート、トリジンジイソシアネート、2,2,4-トリメチルヘキサメチレンジイソシアネート、2,4,4-トリメチルヘキサメチレンジイソシアネート、m-テトラメチルキシリレンジイソシアネート、P-テトラメチルキシリレンジイソシアネート、ダイマー酸ジイソシアネート等のジイソシアン酸エステル化合物と、水酸基、カルボキシル基、アミド基含有ビニルモノマーとを等モルで反応せしめた化合物も、使用することができる。
トリメチレンジイソシアネート、テトラメチレンジイソシアネート、ヘキサメチレンジイソシアネート、ペンタメチレンジイソシアネート、1,2-プロピレンジイソシアネート、2,3-ブチレンジイソシアネート、1,3-ブチレンジイソシアネート、ドデカメチレンジイソシアネート、2,4,4-トリメチルヘキサメチレンジイソシアネート等の脂肪族ジイソシアネート、
ω,ω’-ジイソシアネート-1,3-ジメチルベンゼン、ω,ω’-ジイソシアネート-1,4-ジメチルベンゼン、ω,ω’-ジイソシアネート-1,4-ジエチルベンゼン、1,4-テトラメチルキシリレンジイソシアネート、1,3-テトラメチルキシリレンジイソシアネート等の芳香脂肪族ジイソシアネート、
3-イソシアネートメチル-3,5,5-トリメチルシクロヘキシルイソシアネート[別名:イソホロンジイソシアネート]、1,3-シクロペンタンジイソシアネート、1,3-シクロヘキサンジイソシアネート、1,4-シクロヘキサンジイソシアネート、メチル-2,4-シクロヘキサンジイソシアネート、メチル-2,6-シクロヘキサンジイソシアネート、4,4’-メチレンビス(シクロヘキシルイソシアネート)、1,3-ビス(イソシアネートメチル)シクロヘキサン、1,4-ビス(イソシアネートメチル)シクロヘキサン等の脂環族ジイソシアネートが挙げられる。
具体的には、前記イソシアネート基含有化合物のイソシアネート基を、ε-カプロラクタム、メチルエチルケトン(以下、MEKとも称する)オキシム、シクロヘキサノンオキシム、ピラゾール、フェノール等でブロックしたものなどが挙げられる。特に、イソシアヌレート環を有し、MEKオキシムやピラゾールでブロックされたヘキサメチレンジイソシアネート三量体は、本開示に使用した場合、耐熱性に優れるため、非常に好ましい。また、耐熱性の観点から、イソシアネート基含有化合物(B-3)は、3官能以上のイソシアネート基を有していることが好ましい。
金属キレート化合物(B-4)は、金属と有機物とからなる有機金属化合物であり、バインダー樹脂(A)の反応性官能基と反応して架橋を形成するものである。有機金属化合物の種類は特に限定されないが、有機アルミニウム化合物、有機チタン化合物、有機ジルコニウム化合物などが挙げられる。また、金属と有機物の結合は、金属-酸素結合でもよく、金属-炭素結合に限定されるものではない。加えて、金属と有機物の結合様式は、化学結合、配位結合、イオン結合のいずれであってもよい。更に、前記有機金属化合物は、3官能以上であることが、耐熱性の観点から好ましい。
これらの中でも、金属キレート化合物(B-4)は、有機チタン化合物、または有機ジルコニウム化合物であることが、熱硬化反応性の点から好ましい。
カルボジイミド基含有化合物(B-5)は、分子内にカルボジイミド基を有するものであれば、特に限定されない。カルボジイミド基含有化合物(B-5)としては、例えば、カルボジライトV-01、V-03、V-05、V-07、V-09(商品名、日清紡ケミカル株式会社)、環状カルボジイミド(帝人株式会社)などが挙げられる。耐熱性の観点から、カルボジイミド基含有化合物(B-5)は、1分子中に平均3個以上のカルボジイミド基を有することが好ましい。
次に、本開示で用いるフィラー(C)について詳細に説明する。本接着性樹脂シートは、5%重量分解温度を上げ、はんだリフロー工程後のマイグレーション耐性を向上させる観点から、フィラー(C)を含むことが好ましい。
フィラー(C)としては、例えば、ポリテトラフルオロエチレン粉末やその変性物、テトラフルオロエチレン-パーフルオロアルキルビニルエーテル粉末、テトラフルオロエチレン-エチレン粉末、テトラフルオロエチレン-ヘキサフルオロプロピレン粉末、テトラフルオロエチレン-フッ化ビニリデン粉末、テトラフルオロエチレン-ヘキサフルオロプロピレン-パーフルオロアルキルビニルエーテル粉末、ポリクロロトリフルオロエチレン粉末、クロロトリフルオロエチレン-エチレン粉末、クロロトリフルオロエチレン-フッ化ビニリデン粉末、ポリフッ化ビニリデン粉末、ポリフッ化ビニル粉末等のフッ素系フィラー;
ポリエチレン粉末、ポリアクリル酸エステル粉末、エポキシ樹脂粉末、ポリアミド粉末、ポリイミド粉末、ポリウレタン粉末、液晶ポリマー、ポリシロキサン粉末等の他、シリコーン、アクリル、スチレンブタジエンゴム、ブタジエンゴム等を用いた多層構造のコアシェル等の高分子フィラー;
リン酸メラミン、ポリリン酸メラミン、リン酸グアニジン、ポリリン酸グアニジン、リン酸アンモニウム、ポリリン酸アンモニウム、リン酸アミドアンモニウム、ポリリン酸アミドアンモニウム、リン酸カルバメート、ポリリン酸カルバメート等の(ポリ)リン酸塩系化合物、有機リン酸エステル化合物、ホスファゼン化合物、ホスホン酸化合物、ジエチルホスフィン酸アルミニウム、メチルエチルホスフィン酸アルミニウム、ジフェニルホスフィン酸アルミニウム、エチルブチルホスフィン酸アルミニウム、メチルブチルホスフィン酸アルミニウム、ポリエチレンホスフィン酸アルミニウム等のホスフィン酸化合物、ホスフィンオキシド化合物、ホスホラン化合物、ホスホルアミド化合物等のリン系フィラー;
ベンゾグアナミン、メラミン、メラム、メレム、メロン、メラミンシアヌレート、シアヌル酸化合物、イソシアヌル酸化合物、トリアゾール系化合物、テトラゾール化合物、ジアゾ化合物、尿素等の窒素系フィラー;
シリカや中空シリカや多孔質シリカ、マイカ、タルク、カオリン、クレー、ハイドロタルサイト、ウォラストナイト、ゾノトライト、窒化ケイ素、窒化ホウ素、窒化アルミニウム、リン酸水素カルシウム、リン酸カルシウム、ガラスフレーク、水和ガラス、チタン酸カルシウム、セピオライト、硫酸マグネシウム、水酸化アルミニウム、水酸化マグネシウム、水酸化ジルコニウム、水酸化バリウム、水酸化カルシウム、酸化チタン、酸化スズ、酸化アルミニウム、酸化マグネシウム、酸化ジルコニウム、酸化亜鉛、酸化モリブデン、酸化アンチモン、酸化ニッケル、炭酸亜鉛、炭酸マグネシウム、炭酸カルシウム、炭酸バリウム、ホウ酸亜鉛、ホウ酸アルミニウム等の無機フィラー等が挙げられる。
この他、本接着性樹脂シートには、目的を損なわない範囲で、任意成分として、更に、エネルギー線吸収剤、染料、顔料、酸化防止剤、重合禁止剤、消泡剤、レベリング剤、イオン捕集剤、保湿剤、粘度調整剤、防腐剤、抗菌剤、帯電防止剤、アンチブロッキング剤、赤外線吸収剤、電磁波シールド剤などを添加することができる。また、レーザー加工性向上の点から、本接着性樹脂シートには、エネルギー線吸収剤を配合することが好ましい。
本開示における接着性樹脂シートの硬化物は、23℃において、(i)測定周波数10GHzでの誘電正接が0.005以下であり、(ii)測定周波数20GHzでの誘電正接が0.007以下であり、かつ、(iii)測定周波数40GHzでの誘電正接が0.01以下である。
誘電正接が上記の数値範囲であることで、電子デバイスにおける電気信号の伝送損失が改善する。
また、電気信号の伝送損失の観点から、上記接着剤層の誘電正接は、23℃、測定周波数20GHzにおいて、0.007以下であり、0.006以下であることが好ましく、0.005以下であることが更に好ましく、0.004以下であることが特に好ましい。
さらに、電気信号の伝送損失の観点から、上記接着剤層の誘電正接は、23℃、測定周波数40GHzにおいて、0.010以下であり、0.008以下であることが好ましく、0.007以下であることが更に好ましく、0.006以下であることが特に好ましい。
なお、これらの各測定周波数における接着剤層の誘電正接は、小さければ小さいほど好ましい。
本接着剤層の熱安定性は、JIS K7120で規定された熱重量測定方法に準拠した測定法によって求めることができる。本接着性樹脂シートを180℃で1時間加熱して得られる本接着剤層は、以下の(iv)の条件を満たす。すなわち、(iv)JISK 7120に規定された熱重量測定に準拠し、流入ガス:窒素、測定温度範囲:25℃~500℃、加熱速度:10℃/分、にて測定した質量減少率が5%であるときの温度(以降、5%重量分解温度とも称する)が280℃以上である。本明細書での5%重量分解温度とは、測定前の接着剤層の重量を100%したとき、昇温によって重量が5%減少した時点での温度と定義する。本接着剤層の5%重量分解温度が280℃以上であることで、本接着性樹脂シートの適用例、および本開示の別態様であるプリント配線板の電子部品実装工程のひとつであるはんだリフロー工程での揮発成分(アウトガス)を低減することができる。また、アウトガスの加熱膨張に伴う層間剥離や発泡(フクレ)といった現象を抑制することができ、はんだリフロー工程後のマイグレーション耐性が向上する。同様の観点から、本接着剤層の5%重量分解温度は、290℃以上が好ましく、300℃以上がより好ましい。また、本接着剤層の5%重量分解温度は、プリント配線板の廃棄処理における焼却効率化の観点から、500℃以下が好ましく、450℃以下がより好ましい。
本接着性樹脂シートの硬化物(接着剤層)のガラス転移温度(Tg)は、0~150℃であることが好ましい。本接着剤層のTgが0℃以上であれば、接着剤層の誘電正接をより低下させることができる。また、同様の観点から、本接着剤層のTgは、40℃以上がより好ましく、70℃以上が更に好ましい。本接着剤層のTgが150℃以下であれば、接着剤層の屈曲性をより良好なものとできる。また、同様の観点から、本接着剤層のTgは、120℃以下がより好ましく、100℃以下が更に好ましい。
次に、本接着剤層のTgの求め方について説明する。本接着剤層のTgは、DVA法(動的粘弾性分析法)測定装置等を使用して測定することができる。当該装置によって得られた接着剤層についての粘弾性曲線から、各温度の貯蔵弾性率/損失弾性率の比(tanδ)を求めることができ、tanδ曲線が極大点となる点を、本接着剤層のTgとして求めることができる。なお、tanδ曲線において極大点が複数存在する場合は最も高い極大点を、本接着剤層のTgとする。本接着剤層のTgは、バインダー樹脂(A)のガラス転移温度、硬化剤(B)の量により制御することができる。
本接着性樹脂シートの製造方法は、特に限定されないが、例えば、以下の方法を採用できる。まず、バインダー樹脂(A)と、硬化剤(B)と、フィラー(C)と、その他任意成分と、溶剤とを含む塗布用溶液を、剥離フィルムの片面に塗布する。続いて、前記塗布用溶液に含まれている有機溶剤等の液状媒体を、通常40~150℃で、除去および乾燥し、接着性樹脂シートを形成する。なお、得られた接着性樹脂シートの表面に、別の剥離フィルムを積層することにより、両面剥離フィルム付き接着性樹脂シートを作製してもよい。接着性樹脂シートの両面を剥離フィルムで積層することにより、接着性樹脂シートの表面汚染を予防することができる。なお、剥離フィルムを剥がすことによって、接着性樹脂シートを単離することができる。
2つの剥離フィルムは、同種および異種のもののいずれも用いることができる。また、剥離性の異なる剥離フィルムを接着性樹脂シートの両面に用いることによって、剥離力に強弱をつけることができるので、使用の際に順番に剥がしやすくなる。
本接着性樹脂シート等を用いて、銅張積層板やプリント配線板を得ることができる。言い換えると、本接着性樹脂シートは、銅張積層板用やプリント配線板用として使用することができる。また、これらについて以下に詳しく説明する。
銅張積層板は、銅箔と絶縁性フィルムとが、本接着性樹脂シートの硬化物である接着剤層を介して積層されたものである。
このような銅張積層板は、例えば、以下の方法により得ることができる。すなわち、剥離フィルム付き接着性樹脂シートから剥離性フィルムを順次剥がし、接着性樹脂シート各面に銅箔と絶縁性フィルムとをそれぞれ重ねる(この工程を仮接着とも称する)。続いて、得られた積層体を、加熱もしくは熱プレス工程に処して、銅箔と絶縁性フィルムとの間の接着性樹脂シートを熱硬化することにより、前記銅張積層板を得ることができる。
あるいは、以下の方法により、銅張積層板を得ることもできる。絶縁性フィルム上に接着性樹脂シート形成用の塗布用溶液を塗布および乾燥し、形成された接着性樹脂シート上に銅箔を重ね、加熱もしくは熱プレス工程を経ることにより、銅箔と絶縁性フィルムとの間の接着性樹脂シートを熱硬化することにより、銅張積層板を得ることもできる。
銅張積層板は、銅箔/接着剤層/絶縁性フィルム/接着剤層/銅箔のように、両面最外層をともに銅箔としてもよいし、さらに、銅箔の内層を設けることもできる。複数の接着性樹脂シートを利用して、銅箔や絶縁性フィルムを積層する場合、仮接着を複数回経た後に、複数の接着性樹脂シートの加熱硬化を1度に行うこともできる。
本開示におけるプリント配線板(以降、本プリント配線板とも称する)は、本接着性樹脂シートの硬化物を含む。
例えば、上述した銅張積層板における銅箔をエッチング等によって加工し、信号回路やグランド回路を形成することで、本プリント配線板を得ることができる。また、剥離フィルム付き接着性樹脂シートから剥離フィルムを剥がし、接着性樹脂シート面を回路面に貼り合せ、加熱硬化することで、信号回路を保護したり、更なる多層化のための基体として利用したりすることもできる。
信号回路やグランド回路を設ける方法としては、例えば、以下の方法を用いることができる。まず、上記銅張積層板における銅箔上に、感光性エッチングレジスト層を形成し、回路パターンを持つマスクフィルムを通して露光させて、露光部のみを硬化させる。次いで、未露光部の銅箔をエッチングにより除去した後、残っているレジスト層を剥離するなどして、銅箔から導電性回路を形成することができる。
例えば、ポリエステルやポリイミド、液晶ポリマー、PTFEフィルム等のフレキシブル性、絶縁性のあるプラスチックフィルム上に、導体パターンをプリント技術によって形成する。その後、導体パターンを覆うように、本接着性樹脂シートを介して保護層を重ね、加熱および加圧することによって、接着性樹脂シートを硬化させ、保護層を設けたフレキシブルプリント配線板を得ることもできる。
あるいは、フレキシブル性、絶縁性のあるプラスチックフィルム上にスパッタリングやメッキ等の手段で必要な回路のみを設け、以降同様に、本接着性樹脂シートの硬化物を介して保護層が設けられたフレキシブルプリント配線板を得ることもできる。
《バインダー樹脂(A)の酸価》
バインダー樹脂(A)の酸価はJIS K0070に準じて測定した。具体的には、共栓三角フラスコ中に、試料約1gを精密に量り採り、テトラヒドロフラン/エタノール(容量比:テトラヒドロフラン/エタノール=2/1)混合液100mlを加えて溶解した。これに、フェノールフタレイン試液を指示薬として加え、0.1Nアルコール性水酸化カリウム溶液で滴定し、指示薬が淡紅色を30秒間保持した時を、終点とした。酸価は、次式により求めた(単位:mgKOH/g)。
式(1)
酸価(mgKOH/g)=(5.611×a×F)/S
S:試料の採取量(g)
a:0.1Nアルコール性水酸化カリウム溶液の消費量(ml)
F:0.1Nアルコール性水酸化カリウム溶液の力価
重量平均分子量(Mw)の測定は、東ソー株式会社製GPC(ゲルパーミエーションクロマトグラフィー)商品名:「HPC-8020」を用いた。GPCは、溶媒(THF;テトラヒドロフラン)に溶解した物質を、その分子サイズの差によって分離定量する液体クロマトグラフィーである。本測定は、カラムに商品名:「LF-604」(昭和電工株式会社製:迅速分析用GPCカラム:6mmID×150mmサイズ)を直列に2本接続して用い、流量0.6mL/min、カラム温度40℃の条件で行い、重量平均分子量(Mw)の決定はポリスチレン換算で行った。
フィラー(C)の平均粒子径D50は、レーザー回折・散乱法粒度分布測定装置、商品名:LS13320(ベックマン・コールター社製)を使用し、トルネードドライパウダーサンプルモジュールにて測定して得た数値であり、粒子径累積分布における累積値が50%の粒子径である。なお、屈折率の設定は1.6とした。
(A-1):スチレン系エラストマー、商品名:FG1901GT(マレイン酸変性されたスチレン系エラストマー)、酸価10mgKOH/g、重量平均分子量95,000、Tg80℃(クレイトン社製)。
(A-2):ポリイミド樹脂、酸価9mgKOH/g、重量平均分子量45,000、Tg50℃(トーヨーケム社製)
(A-3):ポリアミド樹脂、酸価10.6mgKOH/g、重量平均分子量21,000、Tg55℃(トーヨーケム社製)
(A-4): ポリウレタン樹脂、酸価10mgKOH/g、重量平均分子量120,000、Tg25℃(トーヨーケム社製)
(A-5):ポリエステル樹脂、商品名:バイロン637、酸価5mgKOH/g、重量平均分子量30,000、Tg21℃(東洋紡社製)
(B-1):商品名:YX-8800(グリシジルエーテル型エポキシ樹脂、官能基当量180g/eq、2官能)、三菱ケミカル社製
(B-2):商品名:MIR-3000(ビフェニルアラルキル型マレイミド樹脂、官能基当量275g/eq)、日本化薬社製
(B-3):商品名:TKA-100(イソシアヌレート型イソシアネート化合物、官能基当量:180g/eq、3官能)、旭化成社製
(B-4):商品名:オルガチックスZC-150(有機ジルコニア化合物、官能基当量122g/eq、4官能)、マツモトファインケミカル社製
(B-5):商品名:カルボジライトV―05(カルボジイミド基含有化合物、官能基当量:262g/eq、多官能)、日清紡ケミカル社製
(B-6):商品名:BAPP(ポリアミノ基含有化合物、官能基当量205g/eq、2官能)、セイカ社製
(C-1):商品名:SC2050-MB(シリカ、平均粒子径D50;0.5μm)、アドマテックス社製
(C-2):商品名:SP-2(窒化ホウ素、平均粒子径D50;4.0μm)、デンカ社製
(C-3):商品名:KT-300(フッ素系フィラー、平均粒子径D50;10.0μm)、喜多村社製
(C-4):商品名:E101―S(液晶ポリマー、平均子粒径D50;17.5μm)、住友化学社製
(C-5):商品名:エクソリットOP935(ホスフィン酸アルミニウム塩、平均子粒径D50;2.5μm)、クラリアント社製
(C-6):商品名:H-Tグレード(アルミナ、平均粒子径D50;1.2μm)、トクヤマ社製
<<塗布液の製造>>
固形分換算で、バインダー樹脂(A-1)を100部、硬化剤(B-1)を5部、フィラー(C-1)を10部、容器に仕込み、不揮発分濃度が30%になるように混合溶剤(トルエン:MEK=9:1(質量比))を加え、ディスパーで10分攪拌して塗布液を得た。
得られた塗布液を、ドクターブレードを使用して、乾燥後の厚さが25μmとなるように厚さ50μmの重剥離フィルム(重離型剤がコーティングされたポリエチレンテレフタレート(PET)フィルム)上に均一塗工して、100℃で2分乾燥させた。その後、室温(例えば、25℃)まで冷却し、片面剥離フィルム付き接着性樹脂シートを得た。次いで、得られた片面剥離フィルム付き接着性樹脂シートの接着性樹脂シート面を厚さ50μmの軽剥離フィルム(軽離型剤がコーティングされたポリエチレンテレフタレート(PET)フィルム)に重ね合わせた。そして、重剥離フィルム/接着性樹脂シート/軽剥離フィルムからなる両面剥離フィルム付き接着性樹脂シートを得た。
後述する方法に従って、接着性樹脂シートの硬化物に対して、10GHz、20GHz、40GHzにおける誘電正接、窒素雰囲気下における5%重量分解温度、ガラス転移温度(Tg)を測定した。また後述する方法に従って、接着性樹脂シートを用いてなる積層配線板Aのマイグレーション耐性並びに、屈曲性に関して評価した。評価結果を表1~3に示す。
上記方法で作製した両面剥離フィルム付き接着性樹脂シートを4枚用意し、剥離フィルムをそれぞれ順次剥がし、露出した接着性樹脂シート同士を計4枚重ね合わせ、真空ラミネーター(ニチゴーモートン製、小型加圧式真空ラミネーターV-130(商品名))で貼り合せた。その際、両面の最外面となる剥離フィルムは剥がさずそのままにした。その結果、4枚の接着性樹脂シートからなる、厚さ100μmの接着性樹脂シートが、重剥離フィルムと軽剥離フィルムの間に挟まれた両面剥離フィルム付き接着性樹脂シートを得た。尚、真空ラミネート条件は加熱温度90℃、真空時間60秒、真空到達圧2hPa、圧力0.4MPa、加圧時間60秒で行った。
次いで、両面剥離フィルム付き接着性樹脂シートを180℃、2MPaにて1時間プレスし、剥離フィルムを剥がし、接着性樹脂シートの硬化物を測定用試験片とした。測定用試験片を、23℃相対湿度50%の雰囲気下で24時間以上保管後、同温湿度環境下、エー・イー・ティー社製の誘電率測定装置を用い、空洞共振器法により、測定周波数10GHzにおける誘電正接を求めた。測定周波数20GHz、40GHzにおいては同様の試験片をそれぞれ対応する周波数の共振器を用いて測定を行った。
(測定用の接着剤層の作製)
各実施例、各比較例で使用した塗布液を、ドクターブレードを使用して、乾燥後の厚さが200μmとなるように厚さ50μmの重剥離フィルム(重離型剤がコーティングされたポリエチレンテレフタレート(PET)フィルム)上に均一塗工して100℃で2分乾燥させた。その後、室温(例えば、25℃)まで冷却し、片面剥離フィルム付き接着性樹脂シートを形成した。
次いで、得られた片面剥離フィルム付き接着性樹脂シートの接着性樹脂シート面を厚さ50μmの軽剥離フィルム(軽離型剤がコーティングされたポリエチレンテレフタレート(PET)フィルム)に重ね合わせ、重剥離フィルム/接着性樹脂シート/軽剥離フィルムからなる両面剥離フィルム付き接着性樹脂シートを得た。
得られた両面剥離フィルム付き接着性樹脂シートを、180℃、1時間、2MPaで熱硬化させ、重剥離フィルムと軽剥離フィルムを剥離することで200μmの接着剤層を得た。
得られた接着剤層から5mm×30mmの大きさに切り出した測定用試験片について、動的粘弾性測定装置、商品名:「DVA200」(アイティー計測制御(株)製)を用い、0℃まで冷却後、昇温速度10℃/分で300℃まで昇温させ、振動周波数10Hzで粘弾性を測定した。
得られた粘弾性曲線から貯蔵弾性率を求めると共に、損失弾性率から損失正接(tanδ)を各温度で算出し、プロットを行い、tanδ曲線が極大となる点を算出し、その点をTgとした。尚、極大点が複数存在する場合には、温度が最も高い値をその硬化物のtanδピーク(Tg)とした。
図1A~図1Dを参照して、マイグレーション耐性の評価方法を説明する。
まず、厚さ12μmの銅箔と厚さ25μmのポリイミドフィルムの積層体をエッチング処理した。そして、図1Aの模式的平面図に示す通り、ポリイミドフィルム1上に、ライン/スペース=0.05mm/0.05mmの、カソード電極接続点2pを備えたカソード電極用櫛型信号配線2と、アノード電極接続点3pを備えたアノード電極用櫛型信号配線3とをそれぞれ形成した。
次いで、図1Bの模式的平面図に示す通り、図1Aに示すカソード電極用櫛型信号配線2およびアノード電極用櫛型信号配線3を覆い、カソード電極接続点2p付近およびアノード電極接続点3p付近が露出する程度の大きさに、両面剥離フィルム付き接着性樹脂シートを貼り付けた。具体的には、両面剥離フィルム付き接着性樹脂シートの軽剥離フィルムを剥がした面を、上述した部分に、貼り付け、真空ラミネーターにて仮接着した。その後、接着性樹脂シートの重剥離フィルムを剥離し、その上に、銅箔5aおよび絶縁層5bから構成される銅張積層板5(CCL)を貼り付けた。具体的には、銅張積層板5の絶縁層5bが、硬化前の接着性樹脂シートと接するようにして、真空ラミネーターで仮接着した後、熱プレスにて180℃、1時間、2MPaで熱硬化させ、接着剤層(接着性樹脂シートの硬化物4)の上に片面CCLが配置された評価用積層配線板Aを得た。図1Cに、作製した評価用積層配線板の模式的平面図を示し、図1Dに、図1Cの評価用積層配線板を線分ID-IDで切断した際の模式的断面図を示す。
A:1000時間経過後の抵抗値が1.0×1010Ω以上、かつ、リークタッチ回数が0回である。
B:1000時間経過後の抵抗値が1.0×108Ω以上かつリークタッチ回数が1回であるか、あるいは、1000時間経過後の抵抗値が1.0×108Ω以上、1.0×1010Ω未満かつリークタッチ回数が0回である。
C:1000時間経過後の抵抗値が1.0×107Ω以上かつリークタッチ回数が2回であるか、あるいは、1000時間経過後の抵抗値が1.0×107Ω以上、1.0×108Ω未満かつリークタッチ回数が1回以下である。
D:1000時間経過後の抵抗値が1.0×107Ω未満であるか、または、リークタッチ回数が3回以上である。
作製した両面剥離フィルム付き接着性樹脂シートの軽剥離フィルムを剥がし、ライン/スペース=0.05mm/0.05mmの回路基板上へ真空ラミネートした。その後、マイグレーション耐性の評価と同様の手順で、評価用積層配線板Aを作製した。
この積層配線板Aを、銅張積層板5が外側になるように180度折り曲げて、折り曲げ部位に500gの錘を5秒間載せた後、折り曲げた箇所を元の平面状態に戻して、再び500gの錘を5秒間載せる操作を行い、この操作を折り曲げ回数1回とした。そして、接着剤層4の500g荷重を掛けた折り曲げ部に、クラックが発生するまでの折り曲げ回数をカウントし、以下の基準で評価した。
なお、クラックが発生したかどうかは、積層配線板Aを剃刀で裁断し、その断面を(株)キーエンス製マイクロスコープ、商品名:「VHX-900」で観察することで確認した。
A:5回以上。
B:3回以上、5回未満。
C:2回以上、3回未満。
D:2回未満。
上記、誘電正接測定と同様に作製した接着性樹脂シートの硬化物(接着剤層)に対して、商品名:TGDTA220(セイコーインスツルメンツ社製)を用いて、5%重量分解温度の測定を行った。なお、測定は、JIS K7120に規定された熱重量測定方法に準拠した。具体的には、アルミ製オープンサンプルパンを使用して、試料(接着剤層)5mg、窒素ガス流量エアー毎分200mL、開始温度25℃、昇温速度毎分10℃の条件で実施し、500℃まで測定を行った。
そして得られた結果から、以下の式(2)を用いて、試料の重量変化を計算し、横軸に温度、縦軸に重量変化をプロットして、5%重量変化があった温度を5%重量分解温度とした。
式(2)
重量変化(%)=温度ごとの重量(g)/測定前硬化物の重量(g)×100
得られた5%重量分解温度を下記の評価基準に基づき評価し、接着剤層の耐熱性を評価した。
A:300℃以上。
B:290℃以上、300℃未満。
C:280℃以上、290℃未満。
D:280℃未満。
表1~3に示すように、バインダー樹脂(A)、硬化剤(B)、フィラー(C)の種類や量を変更した以外は、実施例1と同様にして、接着性樹脂シートを得て、同様に評価した。
2 カソード電極用櫛型信号配線
2p カソード電極接続点
3 アノード電極用櫛型信号配線
3p アノード電極接続点
4 接着性樹脂シートの硬化物(接着剤層)
5 銅張積層板
5a 銅箔
5b 絶縁層
Claims (7)
- 180℃で1時間加熱した際、以下の、i、ii、iiiおよびivを満たすことを特徴とする接着性樹脂シート:
i: 23℃において、測定周波数10GHzでの誘電正接が0.005以下である;
ii: 23℃において、測定周波数20GHzでの誘電正接が0.007以下である;
iii: 23℃において、測定周波数40GHzでの誘電正接が0.01以下である;
iv: JIS K7120に規定された熱重量測定に準拠し、流入ガス:窒素、測定温度範囲:25℃~500℃、加熱速度:10℃/分、にて測定した質量減少率が5%であるときの温度が280℃以上である。 - 180℃で1時間加熱した際のガラス転移温度が、0~150℃であることを特徴とする請求項1に記載の接着性樹脂シート。
- バインダー樹脂、硬化剤およびフィラーを含有し、前記フィラーの含有量が、前記接着性樹脂シートの全質量に対して、50質量%以下であることを特徴とする、請求項1または2に記載の接着性樹脂シート。
- 前記フィラーが、フッ素系フィラー、窒化ホウ素、液晶ポリマー、シリカおよびリン系フィラーからなる群より選ばれる少なくとも一種類を含むことを特徴とする請求項3に記載の接着性樹脂シート。
- プリント配線板用であることを特徴とする請求項1~4のいずれかに記載の接着性樹脂シート。
- 請求項1~5のいずれかに記載の接着性樹脂シートの硬化物を有するプリント配線板。
- 請求項6に記載のプリント配線板を具備してなる電子機器。
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JP2016157838A (ja) * | 2015-02-25 | 2016-09-01 | 東洋インキScホールディングス株式会社 | 電磁波シールドシート、電磁波シールド性配線回路基板および電子機器 |
WO2020262579A1 (ja) * | 2019-06-28 | 2020-12-30 | 三菱瓦斯化学株式会社 | 樹脂組成物、樹脂シート、多層プリント配線板、及び半導体装置 |
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