WO2020085316A1 - Feuille adhésive conductrice - Google Patents

Feuille adhésive conductrice Download PDF

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Publication number
WO2020085316A1
WO2020085316A1 PCT/JP2019/041342 JP2019041342W WO2020085316A1 WO 2020085316 A1 WO2020085316 A1 WO 2020085316A1 JP 2019041342 W JP2019041342 W JP 2019041342W WO 2020085316 A1 WO2020085316 A1 WO 2020085316A1
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WO
WIPO (PCT)
Prior art keywords
conductive adhesive
adhesive sheet
film
resin
wiring board
Prior art date
Application number
PCT/JP2019/041342
Other languages
English (en)
Japanese (ja)
Inventor
青柳慶彦
上農憲治
Original Assignee
タツタ電線株式会社
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by タツタ電線株式会社 filed Critical タツタ電線株式会社
Priority to JP2020503827A priority Critical patent/JP6719036B1/ja
Priority to CN201980052189.XA priority patent/CN112534014B/zh
Priority to KR1020217015386A priority patent/KR102571763B1/ko
Publication of WO2020085316A1 publication Critical patent/WO2020085316A1/fr

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    • 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
    • C09J11/00—Features of adhesives not provided for in group C09J9/00, e.g. additives
    • C09J11/02—Non-macromolecular additives
    • C09J11/06—Non-macromolecular additives organic
    • 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
    • C09J167/00—Adhesives based on polyesters obtained by reactions forming a carboxylic ester 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
    • C09J7/20—Adhesives in the form of films or foils characterised by their carriers
    • C09J7/28—Metal sheet
    • 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
    • C09J9/00—Adhesives characterised by their physical nature or the effects produced, e.g. glue sticks
    • C09J9/02—Electrically-conducting adhesives
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
    • H01B1/20—Conductive material dispersed in non-conductive organic material
    • H01B1/22—Conductive material dispersed in non-conductive organic material the conductive material comprising metals or alloys
    • 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
    • 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
    • C09J2301/00—Additional features of adhesives in the form of films or foils
    • C09J2301/30—Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier
    • C09J2301/312—Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier parameters being the characterizing feature

Definitions

  • the present invention relates to a conductive adhesive sheet. More specifically, the present invention relates to a conductive adhesive sheet used for an electromagnetic wave shielding film used by adhering to a printed wiring board.
  • Conductive adhesives are often used in printed wiring boards.
  • an electromagnetic wave shielding film used by adhering to a printed wiring board (hereinafter sometimes simply referred to as “shield film”) is a shield layer such as a metal foil and a conductive adhesive provided on the surface of the shield layer. And a sheet.
  • the conductive adhesive sheet is formed, for example, by applying a conductive adhesive in the form of a sheet on the surface of the shield layer to adhere the shield layer to the surface of the printed wiring board, and to form the ground pattern and the shield layer of the printed wiring board. To conduct.
  • Such a conductive adhesive sheet firmly adheres to the insulating film (coverlay) provided on the surface of the printed wiring board, and has good electrical continuity with the ground pattern exposed through the opening provided in the insulating film. Is required to be secured.
  • shield film having a conductive adhesive sheet for example, those disclosed in Patent Documents 1 and 2 are known.
  • the shield film is used by adhering the exposed conductive adhesive sheet to the surface of the printed wiring board, specifically, the surface of the cover lay provided on the surface of the printed wiring board.
  • the conductive adhesive layer and the printed wiring board are temporarily attached by lamination or the like (sometimes referred to as “temporary fixing” or “temporary attachment”) to form a laminate.
  • the laminate may be heated to a high temperature (for example, 150 to 180 ° C.) and pressurized to cure the conductive adhesive layer (sometimes referred to as “main curing”).
  • a high temperature for example, 150 to 180 ° C.
  • main curing sometimes referred to as “main curing”.
  • the shield film having a conductive adhesive sheet is, for example, a film having a laminated structure of transfer film / insulating layer (protective layer) / metal layer / conductive adhesive sheet (conductive adhesive layer) / separate film (release base material). It has been known.
  • a conductive adhesive composition is applied onto a separate film to form a conductive adhesive layer, and then a laminated structure of [separate film / conductive adhesive layer] is obtained.
  • a laminated body is produced, and the laminated body and a laminated body having a laminated structure of [transfer film / insulating layer / metal layer] are attached to each other so that the conductive adhesive layer and the metal layer are adhered to each other. Lamination method is adopted.
  • the laminating method requires a multi-step process of manufacturing two laminated bodies separately and then bonding the laminated bodies to each other.
  • a method is known in which the respective layers constituting the shield film are sequentially laminated without producing the two laminated bodies separately.
  • a so-called direct coating method is adopted in which a conductive adhesive composition is directly applied onto a shield layer such as a metal layer to form a conductive adhesive layer.
  • the conductive adhesive layer surface of the shield film becomes the attachment surface to the printed wiring board as described above.
  • the higher the smoothness of the surface of the conductive adhesive layer of the shield film the better the adhesion to the printed wiring board.
  • the conductive adhesive layer in the shield film produced by the laminating method is a layer formed by applying the conductive adhesive composition on a separate film, the conductive adhesive layer to be the bonding surface with the wiring board.
  • the surface has a shape in which the surface shape of the separate film is transferred, that is, it is easy to form a conductive adhesive layer having high surface smoothness, and there is a tendency that the adhesiveness to a printed wiring board is excellent.
  • the conductive adhesive layer surface in the shield film produced by the direct coating method the surface shape of the separate film is not a transferred shape, usually the surface of the conductive particles blended in the conductive adhesive layer Part of it is exposed from the surface of the conductive adhesive layer and tends to have an uneven shape.
  • the shield film produced by the direct coating method has a low smoothness on the surface of the conductive adhesive layer which is a surface to be bonded to the printed wiring board, and the adhesiveness to the printed wiring board tends to be poor.
  • the shield film is apt to be displaced with respect to the printed wiring board or is easily detached from the printed wiring board, that is, the temporary fixing property is poor.
  • the present invention has been made in view of the above, and an object of the present invention is to provide a conductive adhesive sheet having good temporary fixing properties even if the surface smoothness is low.
  • the present inventors have found that the peak top temperature of the storage elastic modulus is 120 ° C. or lower, and the average arithmetic surface roughness Ra of the pasted surface is 0.1 ⁇ m or more. It has been found that the sheet can provide a conductive adhesive sheet having good temporary fixing property even if the surface has low smoothness.
  • the present invention has been completed based on these findings.
  • the present invention provides a conductive adhesive sheet having a storage elastic modulus peak top temperature of 120 ° C. or lower and an average arithmetic surface roughness Ra of the pasting surface of 0.1 ⁇ m or more.
  • the conductive adhesive sheet preferably contains a binder component and metal particles.
  • the binder component preferably contains an epoxy resin and a urethane-modified polyester resin.
  • the conductive adhesive sheet further contains a plasticizer.
  • the conductive adhesive sheet further contains an organic phosphorus flame retardant.
  • the present invention also provides a shield film having the above conductive adhesive sheet.
  • the temporary fixing property becomes good even if the surface smoothness is low. Therefore, for example, even when the shield film is produced by the direct coat method, which is excellent in productivity, the temporary fixing property between the shield film and the printed wiring board is good, and the positional deviation at the time of temporary fixing and the printed wiring board is It is hard to drop out.
  • FIG. 3 is a schematic cross-sectional view showing an embodiment of a shield wiring board formed by bonding a shield film and a printed wiring board by main curing.
  • the peak top temperature of the storage elastic modulus of the conductive adhesive sheet of the present invention is 120 ° C or lower. That is, the conductive adhesive sheet of the present invention has a storage elastic modulus peak top at 120 ° C. or lower.
  • the peak top temperature is preferably 115 ° C or lower, more preferably 110 ° C or lower.
  • the peak top temperature is, for example, 40 ° C. or higher, preferably 80 ° C. or higher, more preferably 90 ° C. or higher. Since the peak top temperature of the storage elastic modulus is 120 ° C. or less, the conductive adhesive sheet of the present invention has high flexibility in the environment at the time of temporary fixing, and the smoothness of the bonding surface with the printed wiring board is low.
  • the conductive adhesive sheet of the present invention is excellent in temporary fixing property with the insulating film, and in the main curing, the adhesive may sufficiently fill the opening provided in the insulating film. Also, it has excellent adhesion to the ground pattern surface. Further, when the peak top temperature of the storage elastic modulus is 40 ° C. or higher, the adhesive is hard to cure in an environment near room temperature, and the storage stability of the conductive adhesive sheet becomes good.
  • the conductive surface of the conductive adhesive sheet of the present invention (the surface on the side to be bonded to the printed wiring board) has an average arithmetic surface roughness (Ra) of 0.1 ⁇ m or more, and may be 0.5 ⁇ m or more, It may be 1 ⁇ m or more, or 1.5 ⁇ m or more.
  • Ra surface roughness
  • the Ra is preferably 5 ⁇ m or less, more preferably 3 ⁇ m or less.
  • Ra is 5 ⁇ m or less, the temporary fixing property between the printed wiring board and the conductive adhesive sheet becomes better.
  • the maximum height roughness (Rp) of the sticking surface (the surface on the side to be stuck to the printed wiring board) of the conductive adhesive sheet of the present invention is not particularly limited, but is preferably 20 ⁇ m or less, more preferably 15 ⁇ m. It is the following. When the Rp is 20 ⁇ m or less, the temporary fixing property between the printed wiring board and the conductive adhesive sheet becomes better.
  • the Rp of the conductive adhesive sheet of the present invention is 0.5 ⁇ m or more from the viewpoint that the temporary fixing property between the printed wiring board and the conductive adhesive sheet is good even when the surface smoothness is low. , 1 ⁇ m or more, or 3 ⁇ m or more.
  • the “adhesive sheet” means a sheet-like material having adhesiveness, and any of the adhesive tape, the adhesive film, and the adhesive layer corresponds to the “adhesive sheet”.
  • the conductive adhesive sheet of the present invention preferably contains at least a binder component and conductive particles.
  • Each of the binder component and the conductive particles may be used alone or in combination of two or more.
  • the above-mentioned binder components include thermoplastic resins, thermosetting resins, active energy ray-curable compounds and the like.
  • thermoplastic resin examples include polystyrene resin, vinyl acetate resin, polyester resin, polyolefin resin (for example, polyethylene resin, polypropylene resin composition, etc.), polyimide resin, acrylic resin and the like.
  • the thermoplastic resins may be used alone or in combination of two or more.
  • thermosetting resin examples include phenol resin, epoxy resin, urethane resin, melamine resin, and alkyd resin.
  • the thermosetting resin may be used alone or in combination of two or more.
  • the epoxy resin is not particularly limited, and examples thereof include bisphenol epoxy resin, spiro ring epoxy resin, naphthalene epoxy resin, biphenyl epoxy resin, terpene epoxy resin, glycidyl ether epoxy resin. Examples thereof include resins, glycidyl amine type epoxy resins, novolac type epoxy resins, and the like.
  • Examples of the bisphenol type epoxy resin include bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol S type epoxy resin, and tetrabromobisphenol A type epoxy resin.
  • Examples of the glycidyl ether type epoxy resin include tris (glycidyloxyphenyl) methane and tetrakis (glycidyloxyphenyl) ethane.
  • Examples of the glycidyl amine type epoxy resin include tetraglycidyl diaminodiphenylmethane.
  • Examples of the novolac type epoxy resin include cresol novolac type epoxy resin, phenol novolac type epoxy resin, ⁇ -naphthol novolac type epoxy resin, and brominated phenol novolac type epoxy resin.
  • bisphenol type epoxy resin is preferable, and bisphenol F type epoxy resin is more preferable.
  • the thermosetting resin preferably includes, for example, a first resin having a reactive first functional group and a second resin having a second functional group capable of reacting with the first functional group.
  • the first functional group include an epoxy group, an amide group, a hydroxyl group and the like.
  • the second functional group may be selected according to the first functional group.
  • the first functional group is an epoxy group, it can be a hydroxyl group, a carboxyl group, an epoxy group, an amino group, or the like.
  • the second resin may be an epoxy group-modified polyester resin, an epoxy group-modified polyamide resin, an epoxy group-modified acrylic resin, an epoxy group-modified polyurethane polyurea resin, a carboxyl group.
  • a modified polyester resin, a carboxyl group-modified polyamide resin, a carboxyl group-modified acrylic resin, a carboxyl group-modified polyurethane polyurea resin, a urethane-modified polyester resin, or the like can be used.
  • carboxyl group-modified polyester resin, carboxyl group-modified polyamide resin, carboxyl group-modified polyurethane polyurea resin, and urethane-modified polyester resin are preferable.
  • examples of the second resin include an epoxy group-modified polyester resin, an epoxy group-modified polyamide resin, an epoxy group-modified acrylic resin, an epoxy group-modified polyurethane polyurea resin, a carboxyl group-modified polyester resin, and a carboxyl group.
  • a group-modified polyamide resin, a carboxyl group-modified acrylic resin, a carboxyl group-modified polyurethane polyurea resin, a urethane-modified polyester resin or the like can be used.
  • carboxyl group-modified polyester resin, carboxyl group-modified polyamide resin, carboxyl group-modified polyurethane polyurea resin, and urethane-modified polyester resin are preferable.
  • the active energy ray curable compound is not particularly limited, and examples thereof include a polymerizable compound having at least two radical reactive groups (for example, (meth) acryloyl group) in the molecule.
  • the active energy ray-curable compound may be used alone or in combination of two or more.
  • the binder component is preferably a thermosetting resin, more preferably an epoxy resin and a urethane-modified polyester resin.
  • the shield film and the printed wiring board are more excellent in temporary fixing property, and in the case of the main curing, they are excellent in adhesiveness and adhesion between the shield film and the printed wiring board due to heat curing. Further, it has excellent adhesion reliability under high temperature and high humidity.
  • a curing agent for accelerating the thermosetting reaction may be included as a component of the binder component.
  • the curing agent can be appropriately selected according to the types of the first functional group and the second functional group.
  • the first functional group is an epoxy group and the second functional group is a hydroxyl group
  • the content of the binder component in the conductive adhesive sheet of the present invention is not particularly limited, but is preferably 5 to 60% by mass, more preferably 10 to 50% by mass relative to 100% by mass of the conductive adhesive sheet of the present invention. It is mass%, more preferably 20 to 40 mass%. When the content ratio is 5% by mass or more, the temporary fixing property is more excellent. When the content ratio is 60% by mass or less, the conductive particles can be sufficiently contained.
  • the content ratio of the first resin in the conductive adhesive sheet of the present invention is not particularly limited, but with respect to the total amount of the conductive adhesive sheet of the present invention 100 mass%. , 0.05 to 20% by mass, more preferably 0.5 to 10% by mass, and further preferably 1 to 5% by mass.
  • the content ratio of the second resin in the conductive adhesive sheet of the present invention in this case is not particularly limited, but is preferably 5 to 50 mass% with respect to 100 mass% of the total amount of the conductive adhesive sheet of the present invention, It is more preferably 10 to 40% by mass, and further preferably 15 to 30% by mass.
  • the content of the curing agent in the conductive adhesive sheet of the present invention is 0.01 to 5 relative to 100 parts by mass of the total amount of the first resin and the second resin.
  • the amount is preferably part by mass, more preferably 0.05 to 1 part by mass, still more preferably 0.1 to 0.5 part by mass.
  • the curing of the first resin and the second resin can be appropriately promoted, and the peak top temperature of the storage elastic modulus of the conductive adhesive sheet can be more easily set to 120 ° C. or less. can do.
  • Examples of the conductive particles include metal particles, metal-coated resin particles, carbon filler, and the like.
  • the conductive particles may be used alone or in combination of two or more.
  • Examples of the metal forming the coating portion of the metal particles and the metal-coated resin particles include gold, silver, copper, nickel, zinc, and the like.
  • the above metals may be used alone or in combination of two or more.
  • the metal particles include copper particles, silver particles, nickel particles, silver-coated copper particles, gold-coated copper particles, silver-coated nickel particles, gold-coated nickel particles, and silver-coated alloy particles.
  • the silver-coated alloy particles include silver-coated copper alloy particles in which alloy particles containing copper (for example, copper alloy particles made of an alloy of copper, nickel and zinc) are coated with silver.
  • the metal particles can be produced by an electrolytic method, an atomizing method, a reducing method, or the like.
  • silver particles, silver-coated copper particles, and silver-coated copper alloy particles are preferable as the metal particles.
  • Silver coated copper particles and silver coated copper alloy particles are particularly preferable from the viewpoints of excellent conductivity, suppressing oxidation and aggregation of metal particles, and reducing the cost of metal particles.
  • the shape of the conductive particles may be spherical, flaky (scaly), dendritic, fibrous, or amorphous (polyhedral).
  • the flake shape is preferable from the viewpoint that the resistance value of the conductive adhesive sheet is lower and the shielding property is better.
  • the average particle diameter (D50) of the conductive particles is preferably 1 to 50 ⁇ m, more preferably 3 to 40 ⁇ m.
  • the average particle diameter is 1 ⁇ m or more, the dispersibility of the conductive particles is good, aggregation can be suppressed, and oxidation is difficult.
  • the average particle diameter is 50 ⁇ m or less, the connectivity with the ground pattern becomes good.
  • the content ratio of the conductive particles in the conductive adhesive sheet of the present invention is not particularly limited, but is preferably 5% by mass or more, and more preferably 20% by mass, based on 100% by mass of the conductive adhesive sheet of the present invention.
  • the above is more preferably 40 mass% or more, and particularly preferably 50 mass% or more.
  • the content ratio of the conductive particles is preferably 90% by mass or less, more preferably 80% by mass or less, further preferably 70% by mass or less, and particularly preferably 64% by mass or less.
  • the content ratio is 90% by mass or less, it becomes easier to set the peak top temperature of the storage elastic modulus of the conductive adhesive sheet to 120 ° C or less.
  • the content ratio is preferably 40% by mass or more, and more preferably 50% by mass or more.
  • the conductive adhesive sheet of the present invention may contain a flame retardant.
  • a flame retardant for example, non-halogen flame retardants are preferable in view of environmental problems, and nitrogen flame retardants such as melamine cyanurate and melamine polyphosphate; metal hydrates such as magnesium hydroxide and aluminum hydroxide; phosphoric acid Examples thereof include phosphorus flame retardants such as ester and red phosphorus.
  • the above flame retardants may be used alone or in combination of two or more.
  • organic phosphorus flame retardants are preferable.
  • the adhesive in the conductive adhesive sheet can more fully fill the opening provided in the insulating film in the printed wiring board, and by the main curing Superior in adhesion to the ground pattern surface.
  • the phosphinic acid metal salt may be used as the organic phosphorus flame retardant.
  • the metal salt of phosphinic acid include aluminum trisdiethylphosphinate, aluminum trismethylethylphosphinate, aluminum trisdiphenylphosphinate, zinc bisdiethylphosphinate, zinc bismethylethylphosphinate, zinc bisdiphenylphosphinate, bisdiethylphosphine.
  • Examples thereof include titanyl acid, titanium tetrakisdiethylphosphinate, titanyl bismethylethylphosphinate, titanium tetrakismethylethylphosphinate, titanyl bisdiphenylphosphinate, and titanium tetrakisdiphenylphosphinate.
  • a blend of a metal salt of phosphinic acid (for example, an aluminum salt of organic phosphinic acid) and melamine polyphosphate may be used.
  • the content ratio of the flame retardant (particularly, the organic phosphorus flame retardant) in the conductive adhesive sheet of the present invention is not particularly limited, but is 0.5 to 30 with respect to 100% by mass of the total amount of the conductive adhesive sheet of the present invention.
  • the content is preferably mass%, more preferably 1 to 25 mass%, further preferably 5 to 20 mass%.
  • flame retardancy becomes better and VTM-0 can be realized.
  • the content ratio is 30% by mass or less, the bulk strength of the conductive adhesive sheet can be kept high, and the temporary adhesiveness and the adhesiveness of the printed wiring board are excellent. Moreover, isotropic conductivity is easily realized.
  • the conductive adhesive sheet of the present invention preferably contains a plasticizer.
  • the plasticizer When the plasticizer is included, the peak top temperature of the storage elastic modulus of the conductive adhesive sheet tends to be lower than that when the plasticizer is not included, and it is easy to set the peak top temperature of the storage elastic modulus to 120 ° C or less Becomes
  • the plasticizer may be used alone or in combination of two or more.
  • plasticizer examples include phthalic acid plasticizers, fatty acid plasticizers, phosphoric acid plasticizers, epoxy plasticizers, polyester plasticizers, and the like. Above all, an epoxy plasticizer is preferable from the viewpoint of excellent temporary fixing property of the conductive adhesive sheet and excellent heat resistance.
  • epoxy-based plasticizer examples include epoxidized soybean oil, epoxidized linseed oil, epoxidized castor oil, epoxidized unsaturated oils and fats such as epoxidized linseed oil; epoxidized linseed oil fatty acid butyl, octylepoxy stearate, Epoxidation of epoxy butyl stearate, epoxidized fatty acid monoester, epoxidized oleic acid octyl ester, epoxidized oleic acid decyl ester, epoxy monoester, alkyl epoxy stearate, n-alkyl epoxy stearate, isoalkyl epoxy stearate, etc.
  • Unsaturated fatty acid ester epoxyhexahydrophthalic acid di-2-ethylhexyl, epoxy hexahydrophthalic acid diisodecyl, cycloalkyl epoxy stearate and other epoxy cyclohexane derivatives; epichlorohydrin Conductor, and the like.
  • the content of the plasticizer in the conductive adhesive sheet of the present invention is not particularly limited, but is preferably 0.5 to 50 parts by mass with respect to 100 parts by mass of the total amount of binder components in the conductive adhesive sheet of the present invention.
  • the amount is more preferably 3 to 30 parts by mass, further preferably 5 to 15 parts by mass, and particularly preferably 6 to 10 parts by mass.
  • the content is 0.5 parts by mass or more, the effect of the plasticizer is sufficiently exhibited, and it becomes easier to set the peak top temperature of the storage elastic modulus of the conductive adhesive sheet to 120 ° C. or lower.
  • the content is 50 parts by mass or less, the embeddability in the opening becomes better, and the flame retardant can be prevented from bleeding out.
  • the electrically conductive adhesive sheet of the present invention may contain other components other than the above components within a range that does not impair the effects of the present invention.
  • the other components include components contained in known or commonly used adhesive sheets.
  • the above-mentioned other components include a defoaming agent, a viscosity modifier, an antioxidant, a diluent, an anti-settling agent, a filler, a colorant, a leveling agent, a coupling agent, and a tackifying resin.
  • the other components may be used alone or in combination of two or more.
  • the conductive adhesive sheet of the present invention preferably has isotropic conductivity.
  • the thickness of the conductive adhesive sheet of the present invention can be appropriately selected according to the application.
  • the above-mentioned thickness is, for example, 1 to 50 ⁇ m, preferably 5 to 25 ⁇ m, from the viewpoint that the conductive adhesive sheet of the present invention is suitable for use as a shield film.
  • the thickness is 1 ⁇ m or more, the embeddability in the opening provided in the insulating film of the printed wiring board becomes better.
  • the thickness is 50 ⁇ m or less, it is possible to meet the demand for thinning.
  • the conductive adhesive sheet of the present invention as a bonding film (for example, a bonding film of a reinforcing plate and a printed wiring board), it is, for example, 10 to 70 ⁇ m, preferably 30 to 65 ⁇ m.
  • the release force of the conductive adhesive sheet of the present invention to the polyimide film which is obtained by the following temporary fixing property test, is not particularly limited, but is preferably 0.5 N / 10 mm or more, more preferably 1 N / 10 mm or more, More preferably, it is 3 N / 10 mm or more.
  • the peeling force is 0.5 N / 10 mm or more
  • the temporary fixing property between the conductive adhesive sheet and the printed wiring board becomes better.
  • Temporal fixability test The surface of the conductive adhesive sheet formed on the separate film and the polyimide film are heated and pressed using a pressing machine under the conditions of temperature: 120 ° C., time: 5 seconds and pressure: 0.5 MPa, and temporarily fixed.
  • the opposite side of the polyimide film to which the conductive adhesive sheet is adhered is fixed to a reinforcing plate with a double-sided tape, and peeled at a pulling speed of 50 mm / min at a peeling angle of 180 ° at room temperature, and the peel strength at peeling is maximum. Measure the value.
  • the resistance value of the conductive adhesive sheet of the present invention obtained by the following conductivity test is not particularly limited, but is preferably 500 m ⁇ or less, more preferably 300 m ⁇ or less, and further preferably 100 m ⁇ or less. When the resistance value is 500 m ⁇ or less, the conductivity between the ground pattern of the printed wiring board and the conductive adhesive sheet becomes good.
  • Conductivity test As a printed wiring board, two copper foil patterns simulating a ground pattern were formed on a base member made of a polyimide film, and an insulating adhesive layer and a cover lay made of a polyimide film were formed thereon. A printed wiring board is used. A gold plating layer is provided as a surface layer on the surface of the copper foil pattern.
  • a circular opening having a diameter of 0.8 mm and simulating a ground connection is formed in the coverlay. Then, the conductive adhesive sheet and the printed wiring board are adhered using a press machine under the conditions of temperature: 170 ° C., time: 30 minutes, pressure: 2-3 MPa, and then electrical resistance between two copper foil patterns. Measure the value with an ohmmeter to obtain the resistance value.
  • the peeling force of the conductive adhesive sheet of the present invention from the polyimide film obtained by the following adhesion test is not particularly limited, but is preferably 3 N / 10 mm or more, more preferably 3.5 N / 10 mm or more, further preferably Is 5 N / 10 mm or more.
  • the peeling force is 3 N / 10 mm or more, the adhesiveness between the conductive adhesive sheet after the main curing and the printed wiring board becomes better.
  • thermosetting bonding film The surface of the conductive adhesive sheet formed on the separate film and the polyimide film are heated and pressed using a pressing machine under the conditions of temperature: 170 ° C., time: 3 minutes, pressure: 2 to 3 MPa to peel the separate film, Temporarily attach the thermosetting bonding film to the exposed surface.
  • a polyimide film is also heat-bonded to the opposite surface of the bonding film using a press machine under the conditions of temperature: 170 ° C., time: 3 minutes, pressure: 2-3 MPa, and further heated at 150 ° C. for 1 hour.
  • the opposite side of the polyimide film to which the conductive adhesive sheet is adhered is fixed to a reinforcing plate with a double-sided tape, and peeled at a pulling speed of 50 mm / min at a peeling angle of 180 ° at room temperature, and the peel strength at peeling is maximum. Measure the value.
  • the peeling force of the conductive adhesive sheet of the present invention with respect to the electrolytic nickel gold plating foil which is obtained by the following adhesiveness test, is not particularly limited, but is preferably 2 N / 10 mm or more, more preferably 3 N / 10 mm or more. .
  • the peeling force is 2 N / 10 mm or more, the adhesiveness between the conductive adhesive sheet after the main curing and the printed wiring board becomes better.
  • Electrolytic nickel gold-plated foil of a laminated film in which an electrolytic nickel gold-plated foil is formed on the surface of a conductive adhesive sheet formed on a separate film and the copper foil of a copper foil laminated film (a laminate of copper foil and a polyimide film) The surface is heated and pressed using a press machine under the conditions of temperature: 170 ° C., time: 3 minutes and pressure: 2 to 3 MPa, the separate film is peeled off, and the thermosetting bonding film is temporarily fixed to the exposed surface.
  • the electrolytic nickel gold plating foil side of the same laminated film as the above laminated film was heated and adhered using a press machine under the conditions of temperature: 170 ° C., time: 3 minutes, pressure: 2-3 MPa. Then, heat at 150 ° C. for 1 hour. Then, the opposite surface side of the electrolytic nickel gold-plated foil to which the conductive adhesive sheet is adhered is fixed to a reinforcing plate with a double-sided tape, and peeled at room temperature at a pulling speed of 50 mm / min and a peeling angle of 180 °, and peeling at peeling. Measure the maximum intensity.
  • the resistance value of the conductive adhesive sheet of the present invention which is obtained by the following conductivity test after being left in an environment of a temperature of 85 ° C. and a humidity of 85% RH for 1000 hours, is not particularly limited, but is preferably 1200 m ⁇ or less. , More preferably 800 m ⁇ or less, still more preferably 500 m ⁇ or less.
  • the resistance value is 1200 m ⁇ or less, the storage stability under high temperature and high humidity is excellent, and the adhesion reliability between the ground pattern of the printed wiring board and the conductive adhesive sheet is excellent.
  • the conductive adhesive sheet of the present invention can be manufactured by a known or commonly used manufacturing method.
  • a temporary base material such as a separate film or a base material is coated (coated) with an adhesive composition for forming a conductive adhesive sheet, and if necessary, desolvated and / or partially cured to form the adhesive composition.
  • an adhesive composition for forming a conductive adhesive sheet, and if necessary, desolvated and / or partially cured to form the adhesive composition.
  • the above adhesive composition contains, for example, a solvent in addition to each component contained in the above-mentioned conductive adhesive sheet.
  • a solvent include toluene, acetone, methyl ethyl ketone, methanol, ethanol, propanol, dimethylformamide and the like.
  • the solid content concentration of the adhesive composition is appropriately set according to the thickness of the conductive adhesive sheet to be formed.
  • a known coating method may be used to apply the adhesive composition.
  • a coater such as a gravure roll coater, a reverse roll coater, a kiss roll coater, a lip coater dip roll coater, a bar coater, a knife coater, a spray coater, a comma coater, a direct coater, and a slot die coater may be used.
  • FIG. 1 is a schematic cross-sectional view showing an embodiment of a shield film having a conductive adhesive sheet of the present invention.
  • the shield film 1 shown in FIG. 1 has a transfer film 11, an insulating layer (protective layer) 12, a metal layer 13, a conductive adhesive sheet (conductive adhesive layer) 14, and a separate film 15 in this order.
  • the conductive adhesive sheet 14 is the conductive adhesive sheet of the present invention.
  • Shield film 1 is used by being attached to the surface of a printed wiring board.
  • FIG. 2 is a schematic cross-sectional view showing one embodiment of a temporarily fixed state in which a shield film is attached to the surface of a printed wiring board.
  • the surface of the conductive adhesive sheet 14 exposed by peeling off the separate film 15 of the shield film 1 and the surface of the insulating film (coverlay) 23 of the printed wiring board 2 are bonded to each other to form a shield.
  • the film 1 and the printed wiring board 2 are temporarily fixed.
  • the printed wiring board 2 includes a board body 21, a circuit pattern including a ground pattern 22 provided on a part of one surface of the board body 21, and an insulating film provided so as to cover a part of the ground pattern 22 ( Cover lay) 23.
  • the insulating film 23 has an opening 23a for exposing a part of the ground pattern 22.
  • the ground pattern 22 has a ground connection portion 22a in the opening 23a.
  • the transfer film 11 is peeled from the shield film 1, and the exposed surface of the insulating layer 12 is heated while being pressed, so that the conductive adhesive sheet 14 is fully cured by heating, for example, from the temporarily fixed state shown in FIG. 14 ', and the shield film is bonded to the printed wiring board 2.
  • the conductive adhesive sheet 14 is bonded to the insulating film 23, and the adhesive that constitutes the conductive adhesive sheet 14 fills the opening 23a, and the opening 23a is filled with the above adhesive and grounded.
  • the shield wiring board Y shown in FIG. 3 is formed by adhering to the pattern 22. By filling the opening 23a with the adhesive forming the conductive adhesive sheet 14, the ground pattern 22 and the metal layer 13 are electrically connected.
  • the pressurizing condition and the heating condition in the main curing are appropriately set depending on the type of the conductive adhesive sheet.
  • the conductive adhesive sheet of the present invention can be used for a shield film having no metal layer. It may be used.
  • it may be obtained by directly forming on the surface of the insulating layer of the laminate having the transfer film and the insulating layer in this order (direct coating method), or once the conductive adhesive sheet of the present invention is formed on the separate film.
  • the conductive adhesive sheet of the present invention may be provided on the metal layer or the insulating layer by transferring (bonding) to the surface of the metal layer or the surface of the insulating layer (laminating method).
  • the conductive adhesive sheet of the present invention is excellent in temporary fixing property with a printed wiring board even if it has low smoothness, it can be produced not only by a laminating method in which a bonded surface tends to be smooth but also by a direct coating method. Further, in the laminating method, it is necessary to once form a conductive adhesive sheet on a separate film and transfer it, so that the productivity may be inferior or the thickness may vary, but the direct coating method solves such a problem. That is, the productivity is excellent and the thickness variation can be suppressed.
  • the conductive adhesive sheet surface of the shield film has a separate film, but also in the case of the direct coating method, a separate film is attached to the surface of the conductive adhesive sheet as necessary. May be.
  • a separate film a base film such as polyethylene terephthalate or polyethylene naphthalate, on which a release agent such as silicone or fluorine is applied on the surface in contact with the conductive adhesive sheet, can be used. .
  • the conductive adhesive sheet of the present invention can be used not only as a shield film but also for mounting a conductive (metal) reinforcing plate on a flexible printed wiring board.
  • the compounding amount shown in the table is a relative compounding amount of each component, and is represented by “parts by mass” unless otherwise specified.
  • the “content of plasticizer (PHR)” indicates the content (parts by mass) of the plasticizer with respect to 100 parts by mass of the binder component.
  • a protective layer resin layer having a thickness of 5 ⁇ m was formed by applying the resin composition for a protective layer to the surface of a PET film (thickness: 25 ⁇ m) whose surface was treated with a release agent, using a wire bar and heating and drying. Next, a copper foil having a thickness of 2 ⁇ m produced by rolling was attached to the surface of the protective layer. Next, the above adhesive composition was applied to the surface of the rolled copper foil with a wire bar and then dried at 100 ° C. for 3 minutes to prepare a shield film having a conductive adhesive sheet.
  • Reference example 1 A commercially available shield film (trade name "PC6000U1" manufactured by Tatsuta Electric Wire Co., Ltd.) was used.
  • room temperature tensile tester manufactured by Shimadzu Corporation, Using the product name "AGS-X50S
  • Adhesiveness (polyimide film) A conductive adhesive sheet surface of the shield film and a polyimide film (manufactured by Toray DuPont Co., Ltd., trade name "Kapton 100H", thickness: 25 ⁇ m) were pressed using a press machine at temperature: 170 ° C., time: 3 minutes, pressure : Heat and pressure were applied under the condition of 2 to 3 MPa, the transfer film was peeled off, and the thermosetting bonding film was temporarily fixed to the protective layer surface.
  • a polyimide film (trade name "Kapton 100H” manufactured by Toray DuPont Co., Ltd., thickness: 25 ⁇ m) was used with a press machine at temperature: 170 ° C., time: 3 minutes, pressure: 2 It was heat-bonded under the condition of ⁇ 3 MPa and further heated at 150 ° C. for 1 hour.
  • the opposite side of the polyimide film to which the shield film is adhered is fixed to a reinforcing plate with a double-sided tape, and a pulling speed is measured at room temperature using a tensile tester (manufactured by Shimadzu Corporation, trade name "AGS-X50S"). Peeling was performed at 50 mm / min and a peeling angle of 180 °, and the maximum peel strength at the time of peeling was measured.
  • Adhesion electrolytic nickel gold plating foil
  • a laminated film in which an electrolytic nickel-gold plated foil (ENIG) (thickness: 0.1 ⁇ m) is formed on the surface of a copper foil of a copper foil laminated film (a laminated body of copper foil and a polyimide film) is used.
  • ENIG electrolytic nickel-gold plated foil
  • the evaluation was performed in the same manner as in (4) Evaluation of adhesiveness except that the electrolytic nickel gold plating foil surface was used as the pasting surface.
  • connection resistance value Two copper foil patterns simulating a ground pattern are formed on a base member made of a polyimide film, and a coverlay (insulating film) made of an insulating adhesive layer and a polyimide film is formed on the copper foil pattern. ) was formed on the printed wiring board. A gold plating layer was provided as a surface layer on the surface of the copper foil pattern. The cover lay was formed with a circular opening simulating the ground connection having a diameter a.
  • the shield film produced in each of the examples and comparative examples, or the shield film of the reference example and the printed wiring board were adhered using a press machine under the conditions of temperature: 170 ° C., time: 30 minutes, pressure: 2 to 3 MPa. .
  • the electrical resistance value between the two copper foil patterns was measured with an ohmmeter, and the connectivity between the copper foil pattern and the conductive adhesive sheet was evaluated and used as the connection resistance value.
  • the measurement was performed for each of the diameters a of 0.5 mm, 0.8 mm, 1.0 mm, 1.4 mm, and 1.8 mm.
  • connection resistance value Adhesion reliability under high temperature and high humidity
  • the same printed wiring board as used in (6) Evaluation of connection resistance value was prepared.
  • the cover lay was formed with a circular opening simulating a ground connection having a diameter of 0.8 mm.
  • the shield film produced in each of the examples and comparative examples, or the shield film of the reference example was allowed to stand for 1000 hours in an environment of a temperature of 85 ° C. and a humidity of 85% RH, and then a press machine was used for temperature: 170 ° C., time: It was adhered to a printed wiring board under the conditions of 30 minutes and pressure: 2-3 MPa. After adhering the shield film, the electrical resistance value between the two copper foil patterns was measured with an ohmmeter, and the connectivity between the copper foil pattern and the conductive adhesive sheet was evaluated and used as the connection resistance value.
  • a shield film (Example) having a conductive adhesive sheet of the present invention having a storage elastic modulus peak top temperature of 120 ° C. or lower was produced by a direct coating method, and the smoothness of the surface of the conductive adhesive sheet was compared.
  • the adhesiveness to the polyimide film and the electrolytic nickel gold plating foil is good, and the connection resistance value after adhesion to the printed wiring board has a diameter of the opening of 0 even though it is relatively low. It was sufficiently low at 0.5 mm or more. Also, the adhesive reliability after storage under high temperature and high humidity was excellent.
  • the shielding film of the reference example has high smoothness of the conductive adhesive sheet, good temporary fixing property, and good adhesion to the polyimide film and electrolytic nickel gold plating foil, but after storage under high temperature and high humidity Was inferior in adhesion reliability.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Physics & Mathematics (AREA)
  • Dispersion Chemistry (AREA)
  • Spectroscopy & Molecular Physics (AREA)
  • Engineering & Computer Science (AREA)
  • Inorganic Chemistry (AREA)
  • Adhesive Tapes (AREA)
  • Shielding Devices Or Components To Electric Or Magnetic Fields (AREA)
  • Adhesives Or Adhesive Processes (AREA)
  • Structure Of Printed Boards (AREA)
  • Conductive Materials (AREA)
  • Soft Magnetic Materials (AREA)

Abstract

La présente invention concerne une feuille adhésive conductrice qui présente une bonne aptitude à la liaison provisoire, même en présence d'une faible rugosité de surface. L'invention concerne notamment une feuille adhésive conductrice qui présente une température limite maximale de module d'élasticité de conservation égale ou inférieure à 120 °C, tout en ayant une surface de liaison qui présente une rugosité de surface moyenne arithmétique Ra égale ou supérieure à 0,1 µm. Il est préférable que cette feuille adhésive conductrice contienne un composant liant et des particules métalliques. Il est également préférable que le composant liant contienne une résine époxyde et une résine polyester modifiée à l'uréthane. Il est également préférable que la feuille adhésive conductrice contienne en outre un plastifiant.
PCT/JP2019/041342 2018-10-22 2019-10-21 Feuille adhésive conductrice WO2020085316A1 (fr)

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CN201980052189.XA CN112534014B (zh) 2018-10-22 2019-10-21 导电性接合片
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WO2022097442A1 (fr) * 2020-11-04 2022-05-12 リンテック株式会社 Film adhésif, film adhésif avec feuille de support, corps durci et procédé de production de structure

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JPWO2020085316A1 (ja) 2021-02-15
KR20210080480A (ko) 2021-06-30
JP6995932B2 (ja) 2022-02-04
TWI796476B (zh) 2023-03-21
CN112534014B (zh) 2022-11-08
CN112534014A (zh) 2021-03-19
JP6719036B1 (ja) 2020-07-08
KR102571763B1 (ko) 2023-08-25
JP2020147759A (ja) 2020-09-17
TW202017462A (zh) 2020-05-01

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