Classifications

• • 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
  • H05K3/38—Improvement of the adhesion between the insulating substrate and the metal
  • H05K3/386—Improvement of the adhesion between the insulating substrate and the metal by the use of an organic polymeric bonding layer, e.g. adhesive
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B15/00—Layered products comprising a layer of metal
  • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
  • B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B27/00—Layered products comprising a layer of synthetic resin
  • B32B27/28—Layered products comprising a layer of synthetic resin comprising synthetic resins not wholly covered by any one of the sub-groups B32B27/30 - B32B27/42
  • B32B27/281—Layered products comprising a layer of synthetic resin comprising synthetic resins not wholly covered by any one of the sub-groups B32B27/30 - B32B27/42 comprising polyimides
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B27/00—Layered products comprising a layer of synthetic resin
  • B32B27/28—Layered products comprising a layer of synthetic resin comprising synthetic resins not wholly covered by any one of the sub-groups B32B27/30 - B32B27/42
  • B32B27/288—Layered products comprising a layer of synthetic resin comprising synthetic resins not wholly covered by any one of the sub-groups B32B27/30 - B32B27/42 comprising polyketones
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B27/00—Layered products comprising a layer of synthetic resin
  • B32B27/30—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers
  • B32B27/302—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers comprising aromatic vinyl (co)polymers, e.g. styrenic (co)polymers
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B27/00—Layered products comprising a layer of synthetic resin
  • B32B27/36—Layered products comprising a layer of synthetic resin comprising polyesters
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B27/00—Layered products comprising a layer of synthetic resin
  • B32B27/38—Layered products comprising a layer of synthetic resin comprising epoxy resins
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B7/00—Layered products characterised by the relation between layers; Layered products characterised by the relative orientation of features between layers, or by the relative values of a measurable parameter between layers, i.e. products comprising layers having different physical, chemical or physicochemical properties; Layered products characterised by the interconnection of layers
  • B32B7/04—Interconnection of layers
  • B32B7/12—Interconnection of layers using interposed adhesives or interposed materials with bonding properties
• • 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
  • C09J125/00—Adhesives based on homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by an aromatic carbocyclic ring; Adhesives based on derivatives of such polymers
  • C09J125/02—Homopolymers or copolymers of hydrocarbons
  • C09J125/04—Homopolymers or copolymers of styrene
  • C09J125/08—Copolymers of styrene
  • C09J125/14—Copolymers of styrene with unsaturated esters
• • 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
  • C09J163/00—Adhesives based on epoxy resins; Adhesives based on derivatives of epoxy resins
• • 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
  • C09J171/00—Adhesives based on polyethers obtained by reactions forming an ether link in the main chain; Adhesives based on derivatives of such polymers
• • 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
  • C09J7/20—Adhesives in the form of films or foils characterised by their carriers
  • C09J7/22—Plastics; Metallised plastics
• • 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
  • 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
  • C09J7/35—Heat-activated
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B2307/00—Properties of the layers or laminate
  • B32B2307/30—Properties of the layers or laminate having particular thermal properties
  • B32B2307/306—Resistant to heat
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B2307/00—Properties of the layers or laminate
  • B32B2307/30—Properties of the layers or laminate having particular thermal properties
  • B32B2307/306—Resistant to heat
  • B32B2307/3065—Flame resistant or retardant, fire resistant or retardant
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B2307/00—Properties of the layers or laminate
  • B32B2307/50—Properties of the layers or laminate having particular mechanical properties
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B2307/00—Properties of the layers or laminate
  • B32B2307/50—Properties of the layers or laminate having particular mechanical properties
  • B32B2307/546—Flexural strength; Flexion stiffness
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B2307/00—Properties of the layers or laminate
  • B32B2307/70—Other properties
  • B32B2307/714—Inert, i.e. inert to chemical degradation, corrosion
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B32—LAYERED PRODUCTS
  • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
  • B32B2457/00—Electrical equipment
  • B32B2457/08—PCBs, i.e. printed circuit boards
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
  • C08G2650/00—Macromolecular compounds obtained by reactions forming an ether link in the main chain of the macromolecule
  • C08G2650/28—Macromolecular compounds obtained by reactions forming an ether link in the main chain of the macromolecule characterised by the polymer type
  • C08G2650/56—Polyhydroxyethers, e.g. phenoxy resins
• • 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
  • C08K5/00—Use of organic ingredients
  • C08K5/0008—Organic ingredients according to more than one of the "one dot" groups of C08K5/01 - C08K5/59
  • C08K5/0066—Flame-proofing or flame-retarding additives
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L25/00—Compositions of, homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by an aromatic carbocyclic ring; Compositions of derivatives of such polymers
  • C08L25/02—Homopolymers or copolymers of hydrocarbons
  • C08L25/04—Homopolymers or copolymers of styrene
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L2666/00—Composition of polymers characterized by a further compound in the blend, being organic macromolecular compounds, natural resins, waxes or and bituminous materials, non-macromolecular organic substances, inorganic substances or characterized by their function in the composition
  • C08L2666/02—Organic macromolecular compounds, natural resins, waxes or and bituminous materials
  • C08L2666/04—Macromolecular compounds according to groups C08L7/00 - C08L49/00, or C08L55/00 - C08L57/00; Derivatives thereof
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L2666/00—Composition of polymers characterized by a further compound in the blend, being organic macromolecular compounds, natural resins, waxes or and bituminous materials, non-macromolecular organic substances, inorganic substances or characterized by their function in the composition
  • C08L2666/02—Organic macromolecular compounds, natural resins, waxes or and bituminous materials
  • C08L2666/14—Macromolecular compounds according to C08L59/00 - C08L87/00; Derivatives thereof
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L33/00—Compositions of homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and only one being terminated by only one carboxyl radical, or of salts, anhydrides, esters, amides, imides or nitriles thereof; Compositions of derivatives of such polymers
  • C08L33/04—Homopolymers or copolymers of esters
  • C08L33/06—Homopolymers or copolymers of esters of esters containing only carbon, hydrogen and oxygen, which oxygen atoms are present only as part of the carboxyl radical
  • C08L33/062—Copolymers with monomers not covered by C08L33/06
  • C08L33/066—Copolymers with monomers not covered by C08L33/06 containing -OH groups
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L63/00—Compositions of epoxy resins; Compositions of derivatives of epoxy resins
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L77/00—Compositions of polyamides obtained by reactions forming a carboxylic amide link in the main chain; Compositions of derivatives of such polymers
• • 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
  • C09J2203/00—Applications of adhesives in processes or use of adhesives in the form of films or foils
• • 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
  • C09J2203/00—Applications of adhesives in processes or use of adhesives in the form of films or foils
  • C09J2203/326—Applications of adhesives in processes or use of adhesives in the form of films or foils for bonding electronic components such as wafers, chips or semiconductors
• • 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
  • C09J2463/00—Presence of epoxy resin
• • 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
  • C09J2477/00—Presence of polyamide
• • 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
  • H05K1/0393—Flexible materials
• • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
  • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
  • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
  • Y10T428/00—Stock material or miscellaneous articles
  • Y10T428/28—Web or sheet containing structurally defined element or component and having an adhesive outermost layer
  • Y10T428/2852—Adhesive compositions
  • Y10T428/287—Adhesive compositions including epoxy group or epoxy polymer

Definitions

• the present invention relates to an adhesive resin composition suitably used for a flexible printed wiring board such as a flexible copper-clad laminate, a flexible printed wiring board using the same, and a laminate such as an adhesive sheet and a coverlay film.
• a flexible printed wiring board (flexible printed wiring board) is based on an insulating film made of a heat-resistant film such as a polyimide film, and copper foil or the like is bonded to one or both surfaces of this insulating film using an adhesive. It is based on a combined structure.
• an adhesive conventionally, an adhesive prepared by blending a flame retardant with a blend resin of an epoxy resin, a phenoxy resin, or the like and a thermoplastic resin such as acrylic, polyamide, or polyester has been used.
• Epoxy resins and phenoxy resins have the role of imparting heat resistance, chemical resistance and mechanical strength, and are thermoplastic.
• the resin has a role of providing high adhesion and flexibility.
• halogen-based flame retardants As a flame retardant, high flame retardancy of VTM-0 class and V-0 class in the UL-94 standard is required. Conventionally, halogen-based flame retardants have been used. However, in recent years, phosphoric acid esters, phosphoric acid ester amides, melamine polyphosphates, ammonium polyphosphates, 9, 10 are used instead of halogen-based flame retardants due to environmental pollution problems. Phosphorus flame retardants such as -dihydro-9-oxa-10-phosphaphenanthrene-10 oxide and its derivatives and phosphazene compounds are used.
• Patent Document 1 Japanese Patent Application Laid-Open No. 2003-176470
• a phosphorus-containing epoxy resin is used, and a phosphorus-containing phenoxy resin is used as a part of the thermoplastic resin so that the phosphorus content in the composition is increased.
• a non-halogen adhesive resin composition having a content of 2% by weight or more has been proposed.
• Patent Document 2 Japanese Patent Application Laid-Open No. 2005-248134 discloses non-halogen-based adhesive resin compositions having excellent flame retardancy as non-halogen-based epoxy resins, polyester resins, acrylic resins, carboxyl group-containing acrylonitrile butadiene rubbers. Adhesive resin compositions using phosphorus-containing compounds such as thermoplastic resins and / or synthetic rubbers, curing agents, phosphate ester compounds, and the like have been proposed.
• Patent Document 3 proposes an adhesive resin composition containing an epoxy resin, a curing agent, and a polymer compound that is incompatible with the epoxy resin.
• a polymer compound incompatible with the epoxy resin an acrylic copolymer having a weight average molecular weight of 100,000 or more containing a functional group such as an epoxy group is used.
• This invention is made
• the place made into the objective is the non-halogen-type adhesive resin composition excellent in the flame retardance, and can obtain the outstanding peeling strength. It is in providing an adhesive resin composition, a laminated body using the same, and a flexible printed wiring board.
• the present inventors impair the compatibility of an epoxy / phenoxy resin with a thermoplastic resin and an epoxy group-containing styrene copolymer by blending a specific amount of an epoxy-containing styrene copolymer.
• the present inventors have found that the adhesion can be greatly improved and completed the present invention.
• the adhesive resin composition of the present invention comprises: (A) an epoxy resin and / or a phenoxy resin; (B) an epoxy-containing styrene copolymer containing an epoxy donor monomer unit and a styrene monomer unit; (D) an adhesive resin composition containing a curing agent, wherein the content of the (B) epoxy-containing styrene copolymer in the total amount of the resin components contained in the resin composition is 3 to 25 mass %.
• the (B) epoxy-containing styrene copolymer preferably has a weight average molecular weight of 5000 to 120,000, and the content of the styrene monomer unit in the (B) is preferably 35 to 98% by mass, and the total amount of resin components The content of the styrene monomer unit is preferably 1 to 20% by mass.
• the (B) epoxy-containing styrene copolymer may further contain an acrylonitrile monomer unit.
• the epoxy equivalent is preferably 250 g / eq or more and 3500 g / eq or less, and the epoxy donor monomer is preferably a (meth) acryl glycidyl ester.
• the (A) epoxy resin and / or phenoxy resin is preferably a phosphorus-containing epoxy resin and / or a phosphorus-containing phenoxy resin from the viewpoint of imparting flame retardancy. Further, it preferably contains a phosphorus-based flame retardant, and the phosphorus content relative to the solid content of the resin composition is 3.1 to 4.5% by mass.
• the laminate of the present invention has an adhesive layer composed of the above-mentioned adhesive resin composition of the present invention on a base film, and a flexible printed wiring board including the laminate is also included in the present invention.
• the adhesive resin composition of the present invention is excellent in compatibility between blended resin components, so it has excellent coating properties and storage stability, and exhibits the desired adhesive strength, mechanical properties, and chemical properties.
• a one-component adhesive solution that can be produced can be provided.
• the adhesive resin composition of the present invention comprises (A) an epoxy resin and / or a phenoxy resin; (B) a styrene copolymer having an epoxy donor monomer unit and a styrene monomer unit; (C) a thermoplastic resin; D) Adhesive resin composition containing a curing agent, wherein the content of the (B) epoxy-containing styrene copolymer in the resin component is within a predetermined range.
• each component will be described in order.
• Epoxy resin and / or phenoxy resin may be a resin having at least two epoxy groups in one molecule, such as bisphenol A type epoxy resin, bisphenol F type epoxy resin, glycidyl.
• examples include ether type epoxy resins, glycidyl ester type epoxy resins, glycidyl amine type epoxy resins, novolac type epoxy resins, cresol novolac type epoxy resins, and the like.
• a bonded phosphorus-containing epoxy resin such as bisphenol A type epoxy resin, bisphenol F type epoxy resin, glycidyl.
• examples include ether type epoxy resins, glycidyl ester type epoxy resins, glycidyl amine type epoxy resins, novolac type epoxy resins, cresol novolac type epoxy resins, and the like.
• Phosphorus-containing epoxy resin can reduce the content of non-halogen flame retardants by demonstrating the flame retardant effect of phosphorus, and as a result, it prevents the decrease in adhesive strength and mechanical strength accompanying flame retardant blending It is preferable because it is possible.
• the phosphorus content increases, the compatibility with other resins tends to deteriorate, so in the case of a phosphorus-containing epoxy resin and a phosphorus-containing phenoxy resin, the amount of the epoxy resin into which phosphorus is incorporated and the respective mass of the phenoxy resin
• the phosphorus content is preferably 2 to 6% by mass.
• phosphorus-containing epoxy resin and phosphorus-containing phenoxy resin examples include FX289, FX305, ERF001 manufactured by Tohto Kasei, and Epicron EXA9710 manufactured by Dainippon Ink & Chemicals, Inc.
• the weight average molecular weight of the epoxy resin and the phenoxy resin is not particularly limited. However, in the epoxy resin, the higher the molecular weight, the worse the compatibility with other resins. The tendency of the phenoxy resin is further increased. Since it is strong, the weight average molecular weight of these resins is preferably determined as appropriate in relation to the compatibility depending on the type used.
• the epoxy resin and phenoxy resin as described above may be used alone or in combination of two or more. Moreover, you may mix and use an epoxy resin and a phenoxy resin.
• the content rate of (A) component in the adhesive resin composition of this invention is not specifically limited, in order to obtain favorable heat resistance, chemical resistance, and mechanical characteristics, the resin component contained in the composition Among them, it is preferable to maximize the content of the component (A).
• the resin component mass contained in the resin composition (the total amount of the component (A), the component (B), the component (C), When other resins are contained, the content is preferably 40 to 70% by mass relative to the amount of the resin added.
• Epoxy-containing styrene-based copolymer (B) Epoxy-containing styrene-based copolymer
• the epoxy-containing styrene-based copolymer used in the present invention is obtained by copolymerizing an epoxy-donating monomer, a styrene-based monomer, and, if necessary, other copolymerizable unsaturated monomers. Is a copolymer.
• the epoxy donor monomer may be any compound having a copolymerizable unsaturated bond and having an epoxy group in the side chain, but preferably a glycidyl group-containing unsaturated monomer is used.
• glycidyl esters of unsaturated carboxylic acids such as glycidyl acrylate, glycidyl methacrylate, monoglycidyl itaconate, butenetricarboxylic acid monoglycidyl ester
• glycidyl such as vinyl glycidyl ether, allyl glycidyl ether, glycidyloxyethyl vinyl ether
• examples include ethers, among which glycidyl acrylate and glycidyl methacrylate are preferably used.
• Styrene monomers include styrene, nucleus-substituted styrene such as o, m, p-methylstyrene, dimethylstyrene, ethylstyrene, and chlorostyrene; styrene such as ⁇ -methylstyrene, ⁇ -chlorostyrene, and ⁇ -chlorostyrene Derivatives are also included. Of these, styrene is preferred.
• copolymerizable unsaturated monomers include, but are not limited to, olefins such as ethylene and propylene; vinyl esters such as vinyl acetate, vinyl propionate and vinyl benzoate; acrylic acid, methacrylic acid, itaconic acid and maleic acid.
• ⁇ , ⁇ unsaturated carboxylic acids or salts thereof such as: methyl (meth) acrylate, ethyl (meth) acrylate, alkyl esters of (meth) acrylic acid such as propyl (meth) acrylate; acrylamide, methacrylamide, etc. Amides; and nitriles such as acrylonitrile.
• These copolymerizable unsaturated monomers are used together with an epoxy-donating monomer and a styrenic monomer as necessary.
• an epoxy-containing styrenic copolymer containing a monomer unit having an amino group or a carboxyl group causes a gradual progress of the curing reaction during storage and may impair the pot life as an adhesive.
• the content of the carboxyl group-containing monomer unit is preferably as small as possible.
• the epoxy-containing styrene copolymer used in the present invention is obtained by copolymerizing the above monomers, and may be a random copolymer of an epoxy donor monomer and a styrene monomer, or the epoxy donor monomer is polymerized. And a block copolymer or a graft copolymer formed by bonding a segment formed by polymerizing a styrene monomer.
• epoxy donor monomers, styrene monomers, and copolymers obtained by random copolymerization of other copolymerizable unsaturated monomers may be used.
• It may be a block copolymer in which a segment formed by polymerization, a segment formed by polymerizing a styrene monomer, and a segment formed by polymerizing other vinyl monomers are appropriately combined, or an epoxy donor monomer is polymerized. And a block copolymer of a segment formed by random copolymerization of a styrene monomer and a vinyl monomer.
• the weight average molecular weight of the epoxy-containing styrene copolymer (B) is not particularly limited, but is preferably about 5000 to 120,000, more preferably 6000 to 90000, and still more preferably 8000 to 28000. If the molecular weight is too high, the compatibility deteriorates and it is difficult to obtain a uniform adhesive solution.
• epoxy-containing styrene-based copolymer (B) In place of the epoxy-containing styrene-based copolymer (B), it is generally carried out in the state of a monomer having excellent compatibility and polymerized by heating. Residual reaction initiators and reaction accelerators are not preferred because of problems in storage stability, such as effects on the properties of the cured product, or reaction that gradually proceeds during storage and gelation. Therefore, it is preferable to use an epoxy-containing styrene copolymer (B) having a weight average molecular weight of 5000 or more that has undergone a certain degree of reaction.
• the epoxy equivalent of the epoxy-containing styrene-based copolymer (B) is preferably 250 g / eq or more and 3500 g / eq or less, more preferably 3000 g / eq or less, and still more preferably 2000 g / eq or less.
• 3500 g / eq although it depends on the molecular weight, the compatibility is deteriorated. As a result, the homogeneity of the adhesive resin composition is lowered, and as a result, the adhesiveness and flame retardancy tend to be lowered.
• the content of the epoxy-donating monomer in the epoxy-containing styrene copolymer (B) depends on the molecular weight of the epoxy-containing styrene copolymer, but it is preferable that the epoxy equivalent is within the above range.
• the content of the styrene monomer unit in the epoxy-containing styrene copolymer (B) is preferably 35 to 98% by mass, more preferably 45 to 96% by mass.
• the content rate of a styrene monomer unit becomes low, it exists in the tendency for the adhesiveness of the adhesive resin composition obtained to fall.
• the content of the styrene-based monomer unit is too high, the content of the epoxy-donating monomer unit becomes relatively small. ), The compatibility with the thermoplastic resin as a component is lowered, and it becomes difficult to prepare a uniform solution type adhesive, resulting in a decrease in adhesiveness.
• the content of the other copolymerizable unsaturated monomer unit is less than 40% by mass. is there.
• acrylonitrile included as another copolymerizable unsaturated monomer, if the amount of acrylonitrile in the copolymerization system is increased, unreacted acrylonitrile monomer tends to remain and is contained in the epoxy-containing styrene copolymer. Since the adverse effect may occur, the content of acrylonitrile in the epoxy-containing styrene copolymer is preferably 1 to 20% by mass, more preferably 1 to 15% by mass.
• epoxy-containing styrene copolymer having the above-described configuration, and examples thereof include Marproof G series from NOF Corporation.
• the (B) epoxy-containing styrenic copolymer having the above-described structure has good compatibility with both the epoxy resin (A) and / or the phenoxy resin and the thermoplastic resin (C). It is possible to provide an adhesive solution having good uniformity and storage stability, and can exhibit high adhesiveness based on the adhesive solution having high uniformity. Furthermore, since the (A) component and a crosslinked structure can be formed by the epoxy group in the (B) epoxy-containing styrene copolymer, excellent mechanical properties can be imparted.
• the content of the (B) epoxy-containing styrenic copolymer in the adhesive resin composition is the total amount of the resin components ((A) component, (B) component, (C) component, etc.) contained in the resin composition, When the resin is included, the amount is 3 to 25% by mass, preferably 3 to 20% by mass, and more preferably 5 to 16% by mass. If it is less than 3% by mass, the effect of improving adhesiveness due to the blending of the epoxy-containing styrene copolymer cannot be obtained. On the other hand, when it exceeds 25% by mass, the compatibility with the component (A) and the component (C) is lowered, and as a result, the storage stability as an adhesive and the adhesive strength are lowered.
• the content rate of the styrene-type monomer unit in (B) epoxy-containing styrene-type copolymer is the resin component amount ((A) component, (B) component, the total amount of (C) component contained in the resin composition,
• the content is preferably 1 to 20% by mass, more preferably 3 to 15% by mass, and still more preferably 4 to 12% by mass with respect to the total amount of the resin.
• thermoplastic resin (C) is not particularly limited.
• Resin polyphenylene sulfide, polyphenylene sulfide ketone, polyphenylene sulfide sulfone, etc.
• polysulfone resin polysulfone, polyether sulfone, etc.
• polyetherimide resin poly-N-formylethyleneimine resin, etc.
• polyether ether ketone resin etc.
• polyacetal Resin polyoxymethylene resin, etc.
• ketone resin aliphatic polyketone resin, acetone formaldehyde resin, acetone furfural resin, cyclic ketone resin, etc.
• thermoplastic resins a polyamide resin is preferably used in consideration of compatibility and adhesion to both (A) an epoxy resin and / or a phenoxy resin and (B) an epoxy-containing styrene copolymer.
• thermoplastic resin in which phosphorus is incorporated in a molecule is preferable because it is excellent in flame retardancy, so that the blending amount of the flame retardant can be reduced and a decrease in adhesive strength accompanying the blending of the flame retardant can be prevented.
• examples of commercially available phosphorus-containing thermoplastic resins include Byron 237, 337, 537, 637 and UR3570 manufactured by Toyobo.
• the polyamide resin can be synthesized by a reaction of dicarboxylic acid, diamine, aminocarboxylic acid, lactam, etc., and is not limited to the reaction of one kind of dicarboxylic acid and diamine, but is synthesized using a plurality of dicarboxylic acids and a plurality of diamines. May be.
• dicarboxylic acid examples include terephthalic acid, isophthalic acid, orthophthalic acid, naphthalenedicarboxylic acid (1,5-, 2,5-, 2,6- and 2,7-isomer) acid, biphenyldicarboxylic acid (2,2 '-, 3,3'- and 4,4'-forms), 4,4'-diphenyl ether dicarboxylic acid, 4,4'-diphenylmethane dicarboxylic acid, 4,4'-diphenylsulfone dicarboxylic acid, 1,2-bis (Phenoxy) ethane-4,4'-dicarboxylic acid, 2,5-anthracene dicarboxylic acid (2,5- and 2,6-isomer), phenylene diacetic acid (o-, m- and p-isomer), Phenylenedipropionic acid (o-, m- and p-isomers), phenylmalonic acid, phenylgluco
• Examples of the diamine include hexamethylenediamine, heptamethylenediamine, p-di-aminomethylcyclohexane, bis (p-aminecyclohexyl) methane, m-xylenediamine, and 1,4-bis (3-aminopropoxy).
• Examples include cyclohexane, piperazine, and isophoronediamine.
• Examples of the aminocarboxylic acid include 11-aminoundecanoic acid, 12-aminododecanoic acid, 4-aminomethylbenzoic acid, 4-aminomethylcyclohexanecarboxylic acid, 7-aminoenanthic acid, 9-aminononanoic acid, and the like. .
• lactam examples include ⁇ -caprolactam, ⁇ -laurolactam, ⁇ -pyrrolidone, ⁇ -piperidone and the like.
• polyamides containing dimer acid as a constituent component can be obtained by a conventional polycondensation of dimer acid and diamine.
• dicarboxylic acid such as adipic acid, azelaic acid or sebacic acid other than dimer acid is used as a co-polymer. You may contain as a polymerization component.
• thermoplastic resin those having a glass transition temperature of 70 ° C. or lower are preferably used. This is because if the glass transition temperature is too high, the handleability is lowered. Moreover, when the glass transition temperature is too high, the adhesiveness tends to decrease.
• (D) Curing agent The curing agent only needs to be used as a curing agent for epoxy resins and phenoxy resins.
• Polyamine curing agents, acid anhydride curing agents, boron trifluoride amine complex salts, imidazole curing agents, Aromatic diamine-based curing agents, carboxylic acid-based curing agents, phenol resins, and the like are used.
• polyamine curing agents include aliphatic amine curing agents such as diethylenetriamine and tetraethylenetetramine; alicyclic amine curing agents such as isophoronediamine; aromatic amine curing agents such as diaminodiphenylmethane and phenylenediamine; dicyandiamide Etc.
• the acid anhydride curing agent examples include phthalic anhydride, pyromellitic acid anhydride, trimellitic acid anhydride, hexahydrophthalic anhydride, and the like.
• curing agent is suitably determined according to the epoxy equivalent of an epoxy resin and / or a phenoxy resin.
• the adhesive resin composition of the present invention comprises an epoxy resin and / or phenoxy resin as the component (A), an epoxy-containing styrene copolymer as the component (B), and a thermoplastic as the component (C).
• thermosetting resins other than other epoxy resins such as phenol resin, melamine resin, and oxazine resin may be added.
• Non-halogen flame retardants that can be used in the present invention include phosphoric acid esters, phosphoric acid ester amides, phosphazenes, and phosphorus such as 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide. System compounds.
• phosphazene is preferably used from the viewpoint of phosphorus concentration and solubility in a solvent.
• Phosphazene is a common name for a compound group having a double bond containing phosphorus and nitrogen as constituent elements, and is not particularly limited as long as it is a compound having a phosphazene structure in the molecule. Cyclophosphazenes having a cyclic structure, chain polymers obtained by ring-opening polymerization thereof, and oligomers may be used.
• the adhesiveness decreases as the content increases, so that it is preferably 30 parts by mass or less per 100 parts by mass of the resin.
• metal hydroxides inorganic fillers
• magnesium hydroxide and aluminum hydroxide as non-halogen flame retardants because they cause a decrease in adhesiveness.
• the adhesive resin composition of the present invention contains the components (A) to (D) as described above and, if necessary, other thermosetting resins, non-halogen flame retardants, and other additives. Prepared. It is preferable to prepare such that the phosphorus content in the adhesive resin composition is 3.1 to 4.5% by mass.
• a curing accelerator In addition, a curing accelerator, a silane coupling agent, a leveling agent, an antifoaming agent, and the like may be appropriately blended.
• a curing accelerator when a curing accelerator is added, the pot life as an adhesive is shortened, and a decrease in adhesiveness is observed. Since it tends to be, it is better not to mix.
• addition of an inorganic filler has the tendency to reduce adhesiveness and a migration characteristic, it is better not to mix
• the adhesive resin composition of the present invention is usually dissolved in an organic solvent and used as an adhesive solution.
• organic solvent include toluene, methanol, ethanol, isopropanol, acetone, dioxolane, hexane, triethylamine, isobutyl acetate, butyl acetate, ethyl acetate, methyl ethyl ketone (MEK), methyl isobutyl ketone, cellosolve, ethylene glycol, dimethylformamide (DMF), Xylene, N-methylpyrrolidone, etc. can be used.
• the solid content concentration in the adhesive solution is preferably 10 to 50% by mass although it depends on the coating method.
• the adhesive resin composition of the present invention having the configuration as described above was uniformly mixed without separation / aggregation of each resin component due to the coexistence of the epoxy-containing styrene copolymer as the component (B).
• a highly adhesive one-component adhesive can be provided.
• the adhesive resin composition of the present invention having the above-described configuration is non-halogen, satisfies UL-94 standard V-0 class and VTM-0 class flame retardancy, and exhibits excellent adhesiveness. Since a solution-type adhesive solution that can be produced can be provided, it is useful as an adhesive for use in laminates such as adhesive sheets and coverlays and flexible printed wiring boards.
• the adhesive resin composition of the present invention is excellent in storage stability as a transparent solution type adhesive, it is suitably used at the production site as a solution type adhesive to be applied on a base film. be able to.
• the flexible printed wiring board is obtained by attaching an insulating film and a metal foil to a plurality of layers with a cured product of the adhesive resin composition of the present invention. That is, the adhesive resin composition of the present invention is applied on an insulating film, dried (semi-cured state), further laminated with a metal foil, and then heat-cured (so-called three-layer substrate); insulating film
• the adhesive resin composition of the present invention is applied and dried (semi-cured state), and the exposed surface of the adhesive layer is covered with an insulating film called a separator (so-called coverlay); on the separator or on the substrate film
• a flexible printed circuit board is formed by coating the adhesive resin composition of the present invention on the substrate, drying it (semi-cured state), laminating the exposed surface covered with a separator (so-called adhesive sheet), etc., and curing by heating. can do. The separator is removed during lamination.
• the semi-cured state is formed by heating the adhesive resin composition of the present invention at, for example, 100 to 180 ° C. for 2 minutes in a state having adhesiveness.
• the heat-cured state is formed by heating a semi-cured adhesive layer at, for example, 140 to 180 ° C. for 10 minutes to several hours, and further pressing as necessary.
• a thermosetting resin epoxy resin
• a suitable heating time varies depending on the component and application of the adhesive (for example, a substrate, a coverlay, or a bonding film).
• the three-layer substrate of the present invention is only required to have a metal foil attached to at least one surface of an insulating film, and has a three-layer structure (so-called three-layer single-sided substrate) comprising an insulating film, an adhesive layer, and a metal foil layer.
• a five-layer structure (so-called three-layer double-sided substrate) composed of a metal foil, an adhesive layer, an electrical insulating film, an adhesive layer, and a metal foil layer may be used.
• Examples of the insulating film include a polyimide film, a polyester film, a polyether ether ketone film, and a polyphenylene sulfide film.
• Examples of the metal foil include copper foil and aluminum foil, and copper foil is preferably used.
• Coverlay film is a laminated body used as a material covering the wiring pattern formation surface to protect the wiring after processing the copper foil of the flexible copper-clad laminate and forming the wiring pattern.
• a semi-cured adhesive layer made of the adhesive resin composition of the present invention is laminated on a film. Usually, a separator having releasability is attached on the adhesive layer.
• the adhesive sheet is a laminate of a separator and, in some cases, a base film and a semi-cured adhesive layer made of the adhesive resin composition of the present invention, and is used for laminating substrates and sticking reinforcing plates. Is called.
• the substrate film may be a prepreg sheet based on a heat-resistant and insulating film such as a polyimide film, a glass fiber reinforced resin sheet, or a nonwoven fabric, depending on the application.
• Adhesive Resin Composition No. Preparation and evaluation of 1 to 13 Mixing polyamide resin (C), phosphorus-containing epoxy / phenoxy resin (A), epoxy-containing styrene copolymer (B) at the ratios shown in Table 1, and adding phosphazene and curing agent as flame retardants Then, it was dissolved in a solvent (methyl ethyl ketone and dimethylformamide) with stirring, and an adhesive solution No. having a solid content concentration of 30% by mass was obtained. 1-13 were prepared.
• a solvent methyl ethyl ketone and dimethylformamide
• phosphorus-containing epoxy / phenoxy resin a 1: 1 mixture of phosphorus-containing epoxy FX289 from Toto Kasei and phosphorus-containing phenoxy ERF001 is used.
• Marproof G0250S molecular weight 20000, epoxy equivalent 310 g / eq, content of styrene monomer unit in epoxy-containing styrene-based copolymer 54 mass%), No.
• Blenmer CP5SA (molecular weight 10000, epoxy equivalent 2500 g / eq, styrene monomer unit content in epoxy-containing styrene copolymer 85 mass%, acrylonitrile monomer unit content 10 mass%) is used. It was. As phosphazene, SPB100 manufactured by Otsuka Chemical was used, and the blending amount was determined so that the phosphorus content relative to the solid content of the adhesive resin composition was 3.5% by mass. As the curing agent, trimellitic acid manufactured by Mitsubishi Chemical Corporation was used, and an appropriate amount calculated from the epoxy equivalent was blended.
• the compatibility decreased as the content of the epoxy-containing styrene copolymer increased.
• the content of the epoxy-containing styrene copolymer is 20% by mass with respect to the resin components (total amount of the components (A), (B), and (C)) in the adhesive resin composition (No. 6)
• the transparency of the adhesive solution is impaired and the content of the epoxy-containing styrene copolymer exceeds 25% by mass (No. 7, 8, 13)
• the adhesive solution is separated into two layers. Therefore, it could not be applied to the base film as it was.
• Adhesive Resin Composition No. Preparation and evaluation of 21-30 An epoxy-containing styrenic copolymer having the characteristics shown in Table 2 is contained at a ratio shown in Table 2, and is stirred and dissolved in a solvent (methyl ethyl ketone and dimethylformamide). . 21 to 28 (the content of the epoxy-containing styrene copolymer in the resin component is 6.7% by mass) was prepared.
• the epoxy-containing styrene copolymer used in Nos. 21 to 25 is a random copolymer of glycidyl methacrylate and styrene.
• the epoxy-containing styrenic copolymers used in Nos. 26 and 27 are terpolymers of glycidyl methacrylate, styrene and acrylonitrile.
• 28 is No. 28.
• No. 21 and epoxy-containing styrenic copolymer used in No. 21. 23 is a 1: 1 mixture of the epoxy-containing styrenic copolymer used in No. 23.
• the adhesive resin composition No. 1 For the polyamide resin, the phosphorus-containing epoxy resin, and the flame retardant, the adhesive resin composition No. 1 was used. For comparison, an adhesive resin composition no. Containing no epoxy-containing styrenic copolymer (B) is used. 29, 30 and No. In the same manner as in No. 21, an adhesive solution was prepared. About the prepared adhesive solution, based on the said evaluation method, compatibility, peeling strength, and a flame retardance were measured and evaluated. The measurement results are shown in Table 2 together with the resin blend composition and the epoxy-containing styrene copolymer characteristics.
• the resin composition (No. 29) that does not contain the epoxy-containing styrene copolymer cannot satisfy the peel strength. Although the peel strength can be increased by reducing the flame retardant content, the degree of improvement is inadequate and the phosphorus content is too low to satisfy the flame retardancy. (No. 30).
• the adhesive resin composition of the present invention is excellent in adhesiveness and flame retardancy, and in the production line, there is a problem of variation in adhesiveness between products, stirring at the start of use, equipment cleaning, etc. It is useful for continuous and intermittent use in production lines without the problem of pot life and storage stability.

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