WO2021024988A1 - 積層体の製造方法 - Google Patents

積層体の製造方法 Download PDF

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Publication number
WO2021024988A1
WO2021024988A1 PCT/JP2020/029687 JP2020029687W WO2021024988A1 WO 2021024988 A1 WO2021024988 A1 WO 2021024988A1 JP 2020029687 W JP2020029687 W JP 2020029687W WO 2021024988 A1 WO2021024988 A1 WO 2021024988A1
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Prior art keywords
polyimide film
film
laminate
protective film
polyimide
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PCT/JP2020/029687
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English (en)
French (fr)
Japanese (ja)
Inventor
真之 熊田
敬太 石山
守 小堺
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株式会社有沢製作所
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Priority to JP2020542922A priority Critical patent/JP7082206B2/ja
Priority to KR1020227003635A priority patent/KR20220044501A/ko
Priority to CN202080056195.5A priority patent/CN114206616A/zh
Publication of WO2021024988A1 publication Critical patent/WO2021024988A1/ja

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    • 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
    • B32B37/00—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding
    • B32B37/10—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the pressing technique, e.g. using action of vacuum or fluid pressure
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C43/00—Compression moulding, i.e. applying external pressure to flow the moulding material; Apparatus therefor
    • B29C43/22—Compression moulding, i.e. applying external pressure to flow the moulding material; Apparatus therefor of articles of indefinite length
    • B29C43/30—Making multilayered or multicoloured articles
    • B29C43/305—Making multilayered articles
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C43/00—Compression moulding, i.e. applying external pressure to flow the moulding material; Apparatus therefor
    • B29C43/32—Component parts, details or accessories; Auxiliary operations
    • B29C43/34—Feeding the material to the mould or the compression means
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C43/00—Compression moulding, i.e. applying external pressure to flow the moulding material; Apparatus therefor
    • B29C43/32—Component parts, details or accessories; Auxiliary operations
    • B29C43/44—Compression means for making articles of indefinite length
    • B29C43/46—Rollers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C43/00—Compression moulding, i.e. applying external pressure to flow the moulding material; Apparatus therefor
    • B29C43/32—Component parts, details or accessories; Auxiliary operations
    • B29C43/52—Heating or cooling
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C63/00—Lining or sheathing, i.e. applying preformed layers or sheathings of plastics; Apparatus therefor
    • B29C63/0065—Heat treatment
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C63/00—Lining or sheathing, i.e. applying preformed layers or sheathings of plastics; Apparatus therefor
    • B29C63/02—Lining or sheathing, i.e. applying preformed layers or sheathings of plastics; Apparatus therefor using sheet or web-like material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/70—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material
    • B29C66/72—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the structure of the material of the parts to be joined
    • B29C66/723—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the structure of the material of the parts to be joined being multi-layered
    • B29C66/7232—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the structure of the material of the parts to be joined being multi-layered comprising a non-plastics layer
    • B29C66/72321—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the structure of the material of the parts to be joined being multi-layered comprising a non-plastics layer consisting of metals or their alloys
    • 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
    • B32B15/088—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 comprising polyamides
    • 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
    • B32B27/34—Layered products comprising a layer of synthetic resin comprising polyamides
    • 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
    • B32B37/00—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding
    • B32B37/04—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the partial melting of at least one layer
    • 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
    • B32B37/00—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding
    • B32B37/06—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the heating method
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C43/00—Compression moulding, i.e. applying external pressure to flow the moulding material; Apparatus therefor
    • B29C43/32—Component parts, details or accessories; Auxiliary operations
    • B29C43/34—Feeding the material to the mould or the compression means
    • B29C2043/3405—Feeding the material to the mould or the compression means using carrying means
    • B29C2043/3422—Feeding the material to the mould or the compression means using carrying means rollers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C43/00—Compression moulding, i.e. applying external pressure to flow the moulding material; Apparatus therefor
    • B29C43/32—Component parts, details or accessories; Auxiliary operations
    • B29C43/34—Feeding the material to the mould or the compression means
    • B29C2043/3483—Feeding the material to the mould or the compression means using band or film carriers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29K—INDEXING SCHEME ASSOCIATED WITH SUBCLASSES B29B, B29C OR B29D, RELATING TO MOULDING MATERIALS OR TO MATERIALS FOR MOULDS, REINFORCEMENTS, FILLERS OR PREFORMED PARTS, e.g. INSERTS
    • B29K2079/00—Use of polymers having nitrogen, with or without oxygen or carbon only, in the main chain, not provided for in groups B29K2061/00 - B29K2077/00, as moulding material
    • B29K2079/08—PI, i.e. polyimides or derivatives thereof
    • 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

Definitions

  • the present invention relates to a method for producing a laminate, and more particularly to a method for producing a laminate in which a polyimide film and a metal foil are laminated.
  • resin layers such as polyimide films and polyamide films having electrical insulation
  • adhesive layers mainly composed of epoxy resin or polyimide resin
  • metal foils such as conductive copper foil, silver foil, and aluminum foil.
  • FPCs flexible printed wiring boards
  • a resin layer is used as a core film (base material), and a metal foil layer is heat-laminated on the surface of the core film via an adhesive layer to obtain a metal-clad laminate.
  • the metal-clad laminate is manufactured by a roll-to-roll method in which each layer is thermocompression-bonded while being continuously conveyed, and the thermal laminate is formed by stacking each layer and passing it between pressure rolls to pass a resin layer and a metal foil.
  • the layer is heated at a temperature equal to or higher than the glass transition temperature (Tg) of the adhesive layer and lower than the melting point, and pressure-bonded.
  • Tg glass transition temperature
  • a flexible copper-clad laminate in which a copper foil is laminated on a polyimide film is generally widely used.
  • the copper foil When producing a copper-clad laminate composed of a polyimide film and a copper foil, in order to improve the adhesion between the polyimide film and the copper foil, the copper foil usually has a fine metal called roughened particles on the surface. A roughening treatment (blackening treatment) for forming particles is performed. However, in the roll-to-roll method, the roughened particles on the surface of the copper foil adhere to the pressure roll, and if the foreign matter is continuously manufactured as it is, the foreign matter is transferred to the surface of the copper foil to form a dent. Sometimes.
  • a method has been proposed in which a protective film is interposed between the copper foil and the pressure roll so that the copper foil does not come into direct contact with the pressure roll.
  • both are placed on at least one surface of a base material made of polyimide, in which a copper foil provided with a rust preventive layer exhibiting a rust preventive effect on the surface of the copper foil layer is placed.
  • a protective film is placed on the surface of at least one of the anticorrosive layers opposite to the copper foil layer at the same time as or prior to laminating by the laminating means and the laminating means.
  • the film sticking means for sticking the rust preventive layer and the protective film while heating to a predetermined temperature and the intermediate product produced by the film sticking means set an appropriate time of 40 to 80 seconds at 200 ° C to 230.
  • Patent Document 2 a film made of a liquid crystal polymer forming an optically anisotropic molten phase and a metal foil are overlapped and passed between pressure rolls to laminate the film and the metal foil.
  • a heating means is provided outside the pressure rolls, and the film and the metal foil and / or the pressure rolls are provided.
  • a method for producing a laminate, which heats or retains heat, is disclosed.
  • Patent Document 1 eliminates waviness when the protective film is peeled off in the rust-preventive copper foil, and does not increase the residual stress in the flexible printed laminated plate.
  • the heat transfer of the pressure roll to the adhesive layer is delayed by the protective film, so that the pressure roll must be sufficiently thermocompression bonded.
  • the transport speed had to be low, and the machining speed was limited.
  • the conventional manufacturing method even when the transport speed is reduced, sufficient heat cannot be applied to the laminate, and the strain remaining inside the polyimide film cannot be sufficiently relaxed. There was a problem.
  • the present invention has been made in view of the above problems, and is a method for producing a laminate for obtaining a flexible metal laminate composed of a polyimide film as a base material and provided with a metal foil, and is a roll-to-roll method.
  • a laminate for obtaining a laminate that can be manufactured at a faster speed than before, has a small variation in dimensional change after etching, and suppresses the occurrence of waviness on the surface of the laminate. It is an object to provide a manufacturing method for the above.
  • the present inventors have identified the polyimide film immediately before the pressure welding portion of the pressure roll when the polyimide film and the metal foil are pressure-bonded between the pressure rolls. By thermocompression bonding while transporting the laminate so as to have a specific temperature range in the above region, and by setting the laminate with the protective film to a specific temperature range in the specific region after the pressure bonding with the pressure roll. We have found that the problem can be solved and have completed the present invention.
  • the present invention is characterized by the following (1) to (7).
  • (1) A method for producing a laminate in which a metal foil is laminated on a polyimide film. While transporting each of the polyimide film, the metal foil and the protective film so as to sandwich the metal foil between at least one surface of the polyimide film and the protective film, the polyimide film, the metal foil and the protective film are transferred. It has a heat crimping step of superimposing each other and hot-bonding the polyimide film and the metal foil between a pair of pressure rolls. In the range of 1 to 200 cm upstream from the pressure contact portion of the pressure roll in the transport direction, the temperature of the polyimide film is set to 70 ° C.
  • the temperature of the laminate with the protective film sent out from the pressure roll is 200 to 350 ° C.
  • Production method. (2) The method for producing a laminate according to (1) above, wherein the temperature of the pressure roll at the time of thermocompression bonding is equal to or higher than the glass transition temperature (Tg) of the polyimide film and 400 ° C. or lower.
  • the polyimide film is heated to 70 ° C. or higher at the time of thermocompression bonding with the pressure roll, so that the surface of the polyimide film is melted in a short time by heating with the pressure roll. It can be integrated with metal foil. Therefore, since the transport speed can be increased, the processing speed can be shortened. Further, if the polyimide film is warmed immediately before crimping with a pressure roll, the distortion inside the polyimide film is alleviated. Therefore, even when manufacturing a single-sided metal leaf laminate, the dimension in the conductor thickness in the laminate is used. The change can be small.
  • FIG. 1 is a diagram showing an outline of a laminated board manufacturing apparatus according to an embodiment of the present invention.
  • FIG. 2 is a diagram for explaining a method of measuring the dimensional change rate.
  • the method for producing a laminate of the present invention is a method for producing a laminate in which a metal foil is laminated on a polyimide film, and the metal foil is sandwiched between at least one surface of the polyimide film and a protective film. It has a thermocompression bonding step in which the films are overlapped with each other and thermocompression bonded between a pair of pressure rolls.
  • the temperature of the polyimide film is set to 70 ° C. or higher and the glass transition temperature of the polyimide film in the range of 1 to 200 cm upstream from the pressure contact portion of the pressure roll in the transport direction.
  • Tg should be less than Tg), and the temperature of the laminate with the protective film sent out from the pressure roll should be 200 to 100 cm in the range of 1 to 100 cm downstream from the pressure contact portion of the pressure roll in the transport direction.
  • the temperature should be 350 ° C.
  • a protective film recovery step of peeling the protective film from the laminate with the protective film carried out from the pressure roll after the thermocompression bonding step it is preferable to have a protective film recovery step of peeling the protective film from the laminate with the protective film carried out from the pressure roll after the thermocompression bonding step.
  • a protective film recovery step of peeling the protective film from the laminate with the protective film carried out from the pressure roll after the thermocompression bonding step.
  • thermocompression bonding process the base material provided with the polyimide film, the metal foil, and the protective film are each pulled out from the supply rolls, conveyed to the pair of pressure rolls, and thermocompression bonded to each other between the pressure rolls. ..
  • the base material is a material that serves as a reinforcing material for the laminate.
  • the base material comprises a polyimide film.
  • the polyimide film includes a layer containing at least a thermoplastic polyimide (thermoplastic polyimide layer), and the thermoplastic polyimide layer is melted by heating and adheres to the metal foil.
  • thermoplastic polyimide layer examples include thermoplastic polyimide, thermoplastic polyamideimide, thermoplastic polyetherimide, and thermoplastic polyesterimide. Of these, thermoplastic polyesterimide is preferable from the viewpoint of low hygroscopicity.
  • the thermoplastic polyimide can be obtained, for example, by copolymerizing an acid dianhydride and a diamine.
  • thermoplastic polyimide examples include pyromellitic dianhydride, 2,3,6,7-naphthalenetetracarboxylic dianhydride, and 3,3', 4,4'-biphenyltetra.
  • thermoplastic polyimide examples include 4,4′-diaminodiphenylpropane, 4,4′-diaminodiphenylmethane, benzidine, 3,3′-dichlorobenzidine, 3,3′-dimethylbenzidine, 2,2.
  • the glass transition temperature (Tg) of the thermoplastic polyimide is not particularly limited because it depends on the use of the flexible metal-clad laminate, but is preferably 240 to 290 ° C, more preferably 260 to 290 ° C, and even more preferably. It is 280 to 290 ° C. When the Tg of the thermoplastic polyimide is 240 ° C. or higher, the bonding with the metal foil tends to be easy, and when the Tg is 290 ° C. or lower, the processability and heat resistance tend to be good.
  • the glass transition temperature (Tg) can be determined from the value of the bending point of the storage elastic modulus measured by a dynamic viscoelasticity measuring device (DMA). For example, "RSA" manufactured by TA Instruments. -G2 "(trade name) is used for measurement at a temperature rise temperature of 10 ° C./min, and the obtained peak of tan ⁇ is defined as Tg (° C.).
  • DMA dynamic viscoelasticity measuring device
  • the coefficient of linear expansion of the thermoplastic polyimide is preferably 20 to 100 ppm / K, more preferably 30 to 70 ppm / K, and even more preferably 40 to 60 ppm / K, from the viewpoint of suppressing dimensional changes in the surface of the laminate. ..
  • the coefficient of linear expansion can be measured by TMA (for example, "TMA-60" (trade name) manufactured by Shimadzu Corporation), and can be obtained in the range of 100 ° C. to 150 ° C. at a heating rate of 10 ° C./min. Obtained from the measured values.
  • the polyimide film preferably includes a layer containing a non-thermoplastic polyimide (non-thermoplastic polyimide layer) in addition to the thermoplastic polyimide layer.
  • non-thermoplastic polyimide refers to a polyimide that does not soften even when heated to 300 ° C. or higher and does not exhibit adhesiveness. By having the non-thermoplastic polyimide layer, heat resistance can be imparted to the laminated body.
  • the non-thermoplastic polyimide used for the non-thermoplastic polyimide layer can be obtained, for example, by copolymerizing an acid dianhydride and a diamine.
  • an acid dianhydride and the diamine any of an aliphatic compound, an alicyclic compound and an aromatic compound can be used, but from the viewpoint of heat resistance, the acid dianhydride is an aromatic tetracarboxylic dianhydride.
  • a compound is preferable, and an aromatic diamine is preferable as the diamine.
  • Examples of the acid dianhydride constituting the non-plastic polyimide include pyromellitic dianhydride, 2,3,6,7-naphthalenetetracarboxylic dianhydride, 3,3', 4,4'-biphenyl.
  • Tetetracarboxylic dianhydride 1,2,5,6-naphthalenetetracarboxylic dianhydride, 2,2', 3,3'-biphenyltetracarboxylic dianhydride, 3,3', 4,4' -Benzophenonetetracarboxylic dianhydride, 3,3', 4,4'-diphenylsulfonetetracarboxylic dianhydride, 4,4'-oxydiphthalic acid dianhydride, 2,2-bis (3,4-di) Carboxyphenyl) propanedianhydride, 3,4,9,10-perylenetetracarboxylic dianhydride, bis (3,4-dicarboxyphenyl) propanedianhydride, 1,1-bis (2,3-di) Carboxiphenyl) ethane dianhydride, 1,1-bis (3,4-dicarboxyphenyl) ethane dianhydride, bis (2,3-dicarboxyphenyl) methan
  • pyromellitic acid dianhydride is mentioned from the viewpoint of heat resistance and dimensional stability.
  • 2,3,6,7-naphthalenetetracarboxylic dianhydride, 2,2', 3,3'-biphenyltetracarboxylic dianhydride, 3,3', 4,4'-biphenyltetracarboxylic acid At least one acid dianhydride selected from the group consisting of dianhydride and 3,3', 4,4'-benzophenonetetracarboxylic dianhydride is preferable.
  • diamine constituting the non-thermoplastic polyimide examples include 4,4'-diaminodiphenylpropane, 4,4'-diaminodiphenylmethane, benzidine, 3,3'-dichlorobenzidine, 3,3'-dimethylbenzidine, 2, 2'-Dimethylbenzidine, 3,3'-dimethoxybenzidine, 2,2'-dimethoxybenzidine, 4,4'-diaminodiphenylsulfide, 3,3'-diaminodiphenylsulfone, 4,4'-diaminodiphenylsulfone, 4 , 4'-oxydianiline, 3,3'-oxydianiline, 3,4'-oxydianiline, 1,5-diaminonaphthalene, 2,6-diaminonaphthalene, 4,4'-diaminodiphenyldiethylsilane, 4,4'-Diaminodiphenylsilane, 4,4'-
  • It preferably contains at least one diamine selected from the group consisting of benzidine, 2,2'-dimethoxybenzidine, 1,5-diaminonaphthalene and 1,4-diaminobenzene (p-phenylenediamine).
  • the glass transition temperature (Tg) of the non-thermoplastic polyimide depends on the use of the flexible metal-clad laminate and is not particularly limited, but is preferably 290 ° C. or higher, more preferably 320 ° C. or higher, and further preferably 340. It is above °C.
  • Tg glass transition temperature
  • the heat resistance tends to be good. Since the higher the Tg of the non-thermoplastic polyimide, the more heat resistant it is, the upper limit thereof is not particularly limited.
  • the coefficient of linear expansion of the non-thermoplastic polyimide is preferably 20 ppm / K or less, more preferably 18 ppm / K or less, still more preferably 16 ppm / K or less, from the viewpoint of suppressing variations in dimensional changes in the surface of the laminate. ..
  • non-thermoplastic polyimide layer a commercially available polyimide film can be used, for example, "Apical NPI” series manufactured by Kaneka Corporation, "Kapton EN” series manufactured by Toray DuPont Co., Ltd., and Ube Industries, Ltd. Examples include the “UPIREX S” series (both are product names).
  • the structure of the polyimide film is not particularly limited as long as the surface in contact with the metal foil is composed of a thermoplastic polyimide layer, for example, a thermoplastic polyimide layer single layer, a thermoplastic polyimide layer / non-thermoplastic polyimide layer, and thermoplastic. Examples thereof include a polyimide layer / a non-thermoplastic polyimide layer / a thermoplastic polyimide layer.
  • the polyimide film is a multilayer film composed of a plurality of layers
  • the polyimide film is a method of heat-bonding each other using a commercially available thermoplastic polyimide film and / or a non-thermoplastic polyimide film as described above, non-thermal. It can be produced by a method of applying a thermoplastic polyimide composition to the surface of a plastic polyimide film and drying it, a method of integrally molding a thermoplastic polyimide composition and a non-thermoplastic polyimide composition, or the like.
  • the coefficient of linear expansion of the entire polyimide film is preferably 10 to 30 ppm / K, more preferably 12 to 25 ppm / K, and 15 to 20 ppm / K from the viewpoint of suppressing variations in dimensional changes within the surface of the laminate. More preferred.
  • polyimide film having a multilayer structure a commercially available product may be used, and for example, "Pixio FRS” series manufactured by Kaneka Corporation and "Yupicel NVT” series manufactured by Ube Industries, Ltd. (both are trade names) are suitable. Listed as a thing.
  • the thickness of the polyimide film is not particularly limited because it depends on the use of the flexible metal-clad laminate, but it is preferably 9 to 75 ⁇ m, more preferably 12. It is 5 to 50 ⁇ m. If the thickness of the polyimide film is less than 9 ⁇ m, the insulating property tends to be inferior, and the mechanical properties such as tearing and tearing tend to be lowered. On the other hand, if the thickness of the polyimide film exceeds 75 ⁇ m, foaming tends to occur easily during the heat treatment, and the flexibility tends to be impaired.
  • the base material may be a single-sided metal-clad laminate in which a metal foil is provided on one side of a polyimide film.
  • Metal foil metals include, for example, copper, aluminum, stainless steel, iron, silver, palladium, nickel, chromium, molybdenum, tungsten, zirconium, gold, cobalt, titanium, tantalum, zinc, lead, tin, silicon, bismuth, indium. Alternatively, these alloys and the like can be mentioned.
  • the structure of the single-sided metal-clad laminate used as the base material is, for example, a thermoplastic polyimide layer / metal foil, a thermoplastic polyimide layer / non-thermoplastic polyimide layer / metal foil, a thermoplastic polyimide layer / non-thermoplastic polyimide layer / heat.
  • a thermoplastic polyimide layer / metal foil examples include a plastic polyimide layer / metal foil.
  • the thickness of the base material is preferably 9 to 75 ⁇ m as described above, and more preferably 12.5 to 50 ⁇ m.
  • the thickness of the entire base material is preferably 10 to 180 ⁇ m, preferably 20 to 70 ⁇ m, in consideration of application to thinning of the flexible metal-clad laminate. More preferred.
  • the metal of the metal foil laminated on the base material is the same as the above-mentioned metal, for example, copper, aluminum, stainless steel, iron, silver, palladium, nickel, chromium, molybdenum, tungsten, zirconium, gold, cobalt, titanium, etc.
  • examples thereof include tantalum, zinc, lead, tin, silicon, bismuth, indium and alloys thereof. Of these, copper or copper alloy metal foils are preferable from the viewpoint of conductivity and circuit processability.
  • the surface of the metal foil may be subjected to an inorganic surface treatment such as galvanization or chrome plating, or an organic surface treatment such as a silane coupling agent.
  • the thickness of the metal foil is not particularly limited because it depends on the use of the flexible metal-clad laminate, but is preferably 1 to 105 ⁇ m, more preferably 9 to 70 ⁇ m, still more preferably 9 to 35 ⁇ m, and most preferably. It is 9 to 18 ⁇ m. If the thickness of the metal foil is less than 1 ⁇ m, circuit defects tend to occur due to pinholes, tears, etc. when the circuit board is manufactured, and if it exceeds 105 ⁇ m, the bonding temperature with the polyimide film becomes high. Productivity tends to decrease.
  • the surface of the metal foil is preferably roughened in order to improve the adhesiveness with the polyimide film of the base material.
  • the surface roughness Rz of the surface of the metal foil in contact with the polyimide film is preferably 0.1 to 0.9 ⁇ m in the case of rolled copper foil, and 0.1 to 1.2 ⁇ m in the case of electrolytic copper foil. It is preferable to have.
  • the surface roughness is 0.1 ⁇ m or more, the adhesive force with the polyimide film tends to be improved.
  • the thickness of the thermoplastic polyimide required to fill the roughness (unevenness) of the copper foil is high. It tends to be thinner and the dimensional change of the laminate tends to be smaller.
  • metal foil for example, "Rolled Copper Foil BHY” series manufactured by JX Nippon Mining & Metals Co., Ltd., “Rolled Copper Foil ROFL” series manufactured by Fukuda Metal Foil Powder Industry Co., Ltd. (both are trade names), etc. Is mentioned as a suitable one.
  • the protective film is a film for interposing between the metal foil and the pressure roll so that the metal foil does not come into direct contact with the pressure roll. Even if foreign matter or the like adheres to the pressure contact surface of the pressure roll, the protective film prevents the foreign matter or the like from coming into contact with the metal foil and prevents the surface of the metal foil from forming a dent due to the foreign matter or the like. it can. Further, by attaching the protective film to the outermost surface of the laminated body, it is possible to suppress rapid cooling of the laminated body after thermocompression bonding and prevent appearance defects such as waviness.
  • any resin film or metal foil that can withstand the heat during lamination can be used, and examples thereof include a non-thermoplastic polyimide film and a polyamide film. Of these, a non-thermoplastic polyimide film having excellent heat resistance is more preferable.
  • the thickness of the protective film is preferably 25 to 125 ⁇ m, more preferably 50 to 125 ⁇ m, and even more preferably 75 to 125 ⁇ m.
  • the thickness of the protective film is 25 ⁇ m or more, it is possible to prevent the foreign matter shape existing on the pressure roll from being transferred to the metal foil at the time of crimping, and the laminate sent out from the pressure roll after thermocompression bonding is rapidly cooled. It is possible to prevent appearance defects such as waviness. If it is 125 ⁇ m or less, the heat of the pressure roll can be sufficiently transferred to the laminated plate at the time of thermocompression bonding.
  • the protective film a commercially available product may be used, and examples thereof include the "Apical NPI” series manufactured by Kaneka Corporation and the “Kapton H” series manufactured by Toray DuPont Co., Ltd. (both are trade names). ..
  • thermocompression bonding step a metal foil is bonded to the thermoplastic polyimide layer of the polyimide film which is the base material.
  • the method of laminating include a method of laminating using a thermal roll laminating apparatus having a pair of pressure rolls.
  • metal foils 2a and 2b and protective films 3a and 3b are placed on both sides of the polyimide film (specifically, thermoplastic polyimide layer / non-thermoplastic polyimide layer / thermoplastic polyimide layer) 1 in this order.
  • Each of them is conveyed to the pressure rolls 7a and 7b so as to be laminated, and the laminated polyimide films 1, metal foils 2a and 2b and the protective films 3a and 3b are combined with the polyimide film 1 between the pressure rolls 7a and 7b.
  • the metal foils 2a and 2b are heat-bonded.
  • the thermal roll laminating apparatus includes a polyimide film supply roll 11 for supplying a polyimide film (base material), metal foil supply rolls 12a and 12b for supplying a metal foil, and a protective film supply for supplying a protective film.
  • the protective film winding rolls 14a and 14b for winding the protective film after the heat-bonding step and the laminate winding roll 16 for winding the laminate are provided.
  • the polyimide film 1, the metal foils 2a, 2b, and the protective films 3a, 3b sent out from each supply roll are placed between the polyimide film 1 and the protective films 3a, 3b via the transport rollers 21a to 21e.
  • the polyimide film 1 and the metal foils 2a and 2b are heat-bonded by being conveyed so as to sandwich the polyimide film 1 and being heated and pressed between the pressure rolls 7a and 7b by overlapping each other.
  • the temperature of the polyimide film 1 in the region R1 immediately before the pressure contact portion 71 of the pressure rolls 7a and 7b in the transport direction is set to 70 ° C. or higher and lower than the glass transition temperature (Tg) of the polyimide film 1. ..
  • the region R1 immediately before being carried into the pressure welding portion 71 is in a range of 1 to 200 cm on the upstream side of the pressure welding portion 71, and the temperature of the polyimide film 1 in this range should be at least 70 ° C. or lower and less than Tg of the polyimide film 1. Therefore, the surface of the polyimide film 1 can be softened to the extent that it does not melt, and the state can be maintained until just before entering the pressure rolls 7a and 7b.
  • the polyimide film 1 and the metal foils 2a and 2b can be bonded to each other in a short time during crimping. Further, if the polyimide film is warmed immediately before crimping with a pressure roll, the distortion inside the polyimide film is alleviated. Therefore, even when manufacturing a single-sided metal leaf laminate, the dimension in the conductor thickness in the laminate is used. The change can be small.
  • the region R1 is preferably in the range of 1 to 220 cm on the upstream side from the pressure contact portion 71, and more preferably in the range of 1 to 250 cm.
  • the temperature of the polyimide film 1 may be at least the temperature of the surface of the polyimide film 1 within the above range.
  • thermoplastic polyimide layer constituting the surface of the polyimide film 1 is 70 ° C. or higher.
  • the temperature should be lower than the glass transition temperature (Tg) of the thermoplastic polyimide layer.
  • Tg glass transition temperature
  • the temperature of the polyimide film 1 in the region R1 is preferably 120 ° C. or higher, more preferably 200 ° C. or higher.
  • the method for adjusting the temperature of the polyimide film 1 in the region R1 is not particularly limited as long as the polyimide film 1 in the region R1 can be maintained at a constant temperature.
  • the polyimide film 1 in the region R1 is heated by a heater or the like.
  • the method of directly heating with hot air, an infrared heater, a ceramic heater or the like has good thermal efficiency and can prevent the heat laminator device from becoming large in size.
  • Examples of the method for measuring the temperature of the polyimide film 1 include a method of measuring in contact with the polyimide film 1 and a method of measuring in a non-contact manner.
  • Examples of the method of measuring in contact with the polyimide film 1 include a method of attaching a thermocouple to the polyimide film 1 conveyed to the region R1 and measuring.
  • Examples of the non-contact measuring method include a method of measuring the polyimide film 1 conveyed to the region R1 with a non-contact thermometer, a method of measuring the ambient temperature in the vicinity of the polyimide film 1 and predicting the temperature of the polyimide film. Be done.
  • non-contact measurement is preferable from the viewpoint of preventing wrinkles and irregularities from being formed on the film due to contact with foreign matter during transportation of the polyimide film 1.
  • the temperature within 15 cm from the upper surface or the lower surface of the polyimide film 1 conveyed in the region R1 is measured, and the temperature obtained by adding about 23 ° C. from that temperature is the temperature of the polyimide film 1. It can be the predicted temperature.
  • the pressure rolls 7a and 7b metal rolls, rubber rolls and the like can be used, and among them, it is preferable to use metal rolls having excellent heat resistance.
  • the metal roll include an iron roll and a stainless steel roll.
  • the temperature of the pressure roll during thermocompression bonding (also referred to as the lamination temperature) is preferably equal to or higher than the glass transition temperature (Tg) of the polyimide film 1 and 400 ° C. or lower.
  • Tg of the polyimide film 1 refers to the temperature of the thermoplastic polyimide layer constituting the surface of the film.
  • the transport speed (also referred to as laminating speed) of the material to be laminated during thermocompression bonding in the thermocompression bonding step can be 2.0 m / min or more. Since the laminating speed is 2.0 m / min or more, the processing speed is high and the laminated body can be mass-produced in a short time. From the viewpoint of the adhesiveness of the laminated body, the laminating speed is preferably 2.0 to 6.0 m / min, more preferably 2.0 to 4.0 m / min.
  • the laminating pressure is preferably in the range of 5 to 50 kN, and more preferably in the range of 10 to 30 kN.
  • the tension applied to the polyimide film 1 at the time of lamination is preferably 0.1 to 20 kg / m, more preferably 0.2 to 15 kg / m, and even more preferably 0. It is 5 to 10 kg / m. If the tension is less than 0.1 kg / m, it tends to be difficult to obtain a laminated body having a good appearance, and if it exceeds 20 kg / m, the dimensional stability tends to be inferior.
  • the laminated body 5 with a protective film that is thermocompression-bonded by the pressure rolls 7a and 7b and sent out from the pressure rolls 7a and 7b is 200 in the region R2 immediately after the pressure contact portion 71 of the pressure rolls 7a and 7b.
  • the temperature should be ⁇ 350 ° C.
  • the region R2 immediately after being carried out from the pressure contact portion 71 is at least in the range of 1 to 100 cm on the downstream side from the pressure contact portion 71, and by setting the temperature of the laminate 5 with the protective film in this range to 200 to 350 ° C., the protective film Since the laminated body 5 can be prevented from being cooled rapidly and the temperature can be gradually lowered, it is possible to suppress the occurrence of poor appearance and variation in dimensional change.
  • the region R2 is preferably in the range of 1 to 120 cm downstream from the pressure contact portion 71, and more preferably in the range of 1 to 150 cm.
  • the temperature of the laminated body 5 with the protective film may be set so that the temperature of the surface thereof is within the above range.
  • the temperature of the protective films 3a and 3b which are the surface layers of the laminated body 5 with the protective film is 200. It is preferable to set the temperature to about 350 ° C.
  • the temperature of the laminated body 5 with the protective film in the region R2 is preferably 250 to 350 ° C., more preferably 280 to 350 ° C.
  • the method for adjusting the temperature of the laminate 5 with the protective film in the region R2 is not particularly limited as long as the laminate with the protective film in the region R2 can be maintained at a predetermined temperature.
  • the laminate with the protective film in the region R2. A method of heating the body 5 using a heating device such as a heater, a method of surrounding the laminated body 5 with a protective film of at least region R2 in a chamber and heating the inside of the chamber using a heating device, etc., and installing a thermal roll laminating device. Examples include a method of heating the entire chamber.
  • the regions R1 and the regions R2 may be surrounded by one chamber together with the pressure rolls 7a and 7b.
  • the method for measuring the temperature of the laminated body 5 with the protective film is the same as described above, and either the contact method or the non-contact method can be adopted.
  • the laminate 5 with a protective film can be obtained as described above, but in the present embodiment, the thermocompression bonding step is preferably performed in an inert gas atmosphere. Oxidation of the metal foil can be suppressed by performing the operation in an atmosphere of an inert gas.
  • the inert gas include nitrogen gas and argon gas.
  • the protective films 3a and 3b are peeled off from the laminate 5 with the protective film, and the protective films 3a and 3b are wound around the protective film winding rolls 14a and 14b via the transport rollers 22a to 22d, and the polyimide film 1 and the metal are wound.
  • the laminate 6 on which the foils 2a and 2b are laminated is wound on the laminate take-up roll 16.
  • the thickness of the laminated body is preferably 30 to 100 ⁇ m.
  • the bendability as an FPC is improved, which is preferable. If the thickness is less than 30 ⁇ m, it may be difficult to handle during processing, and if it exceeds 100 ⁇ m, the bendability as an FPC may be lowered and it may be difficult to reduce the thickness.
  • any number of transport rollers for transporting the material to be laminated and the laminate with the protective film in the thermal roll laminating apparatus can be provided at any place. For example, if a transport roller is placed near the pressure roll and the protective film is transported along the pressure roll, the moisture in the protective film is removed by the heat of the pressure roll, and the metal foil is laminated. There is no risk that air will collect between the film and the protective film and the adhesiveness will deteriorate. Further, if a plurality of transfer rollers are installed immediately after the pressure roll and the laminated body with the protective film is conveyed while being bent, the length of the region R2 occupied in the length direction of the thermal roll laminating device can be shortened. Therefore, it is possible to prevent the device from becoming large.
  • thermocouple was attached to a polyimide film 200 cm upstream from the pressure contact part of the pressure roll of the thermal laminating device, and a PC-link type high-performance recorder (“GR-3500” (trade name) manufactured by KEYENCE CORPORATION) was used. The measurement was performed.
  • PC-link type high-performance recorder (“GR-3500” (trade name) manufactured by KEYENCE CORPORATION) was used. The measurement was performed.
  • thermometer (“THERMO-HUNTER MODEL PT-2LD” (trade name) manufactured by OPTEX) measures the temperature within 15 cm from the upper surface of the laminate with a protective film 100 cm downstream from the pressure contact portion of the pressure roll of the thermal laminating device. ), And the temperature obtained by adding 23 ° C. from that temperature was used as the predicted temperature of the laminate with the protective film.
  • the measurement was performed according to Section 9.6 of JIS C 6471. Specifically, the measurement was performed as follows. As shown in FIG. 2, two samples having substantially the same size were cut out from the flexible copper-clad laminate 6 having a width of 500 mm in the width direction. As shown in FIG. 2, for each of the samples 8A and 8B, two reference points along the length direction are determined, another reference point is determined at a location 195 mm in the width direction from these reference points, and the other reference points are determined in the length direction. The lengths MD-L1 to MD-L4 between the opposing reference points were measured (initial length). The initial lengths MD-L1 to MD-L4 between the reference points were set to 255 mm.
  • the copper foil on the surface of the laminate was removed by etching, and after leaving it in a standard state for 12 hours or more, the lengths MD-L1 to MD-L4 between the reference points were measured again (length after etching).
  • the dimensional change rates of the lengths MD-L1, MD-L2, MD-L3 and MD-L4 between the reference points were calculated according to the following formula.
  • Dimensional change rate (%) (length after etching-initial length) / initial length x 100
  • Example 1 Using a thermal laminating apparatus having a pair of pressure rolls 7a and 7b as shown in FIG. 1, a flexible copper-clad laminate in which a copper foil and a protective film were laminated in this order on both sides of a polyimide film was produced. The device was operated under nitrogen gas. Copper foils 2a and 2b were sandwiched between the polyimide film 1 and the protective films 3a and 3b, and each of them was conveyed at a speed of 4.0 m / min while being overlapped with each other and thermocompression bonded between the pressure rolls 7a and 7b. .. The temperature of the pressure roll was 365 ° C. and the pressure was 21 kN.
  • a heater was installed at a position 200 cm upstream from the pressure contact portion 71 of the pressure rolls 7a and 7b, and heated so that the temperature of the polyimide film at this position was 70 ° C. Then, a heater was installed at a position 100 cm downstream from the pressure contact portion 71 of the pressure rolls 7a and 7b, and the laminate 5 with a protective film at this position was heated so as to have a temperature of 200 ° C. After thermocompression bonding, the protective films 3a and 3b are peeled off from the laminate 5 with the protective film at a position 300 cm downstream of the pressure rolls 7a and 7b, and the flexible copper-clad laminate 6 is wound around the laminate take-up roll 16. I took it. Using the obtained flexible copper-clad laminate, the dimensional change rate and appearance (waviness) were evaluated. The results are shown in Table 1.
  • Example 2 A flexible copper-clad laminate was obtained by the same method as in Example 1 except that the temperature of the polyimide film at a position 200 cm upstream from the pressure contact portion of the pressure roll was heated to 200 ° C. And the appearance (wavy) was evaluated. The results are shown in Table 1.
  • Example 3 A flexible copper-clad laminate was obtained by the same method as in Example 1 except that the temperature of the laminate with the protective film at a position 100 cm downstream from the pressure contact portion of the pressure roll was heated to 250 ° C. The rate of change and appearance (waviness) were evaluated. The results are shown in Table 1.
  • Example 1 A flexible copper-clad laminate was obtained by the same method as in Example 1 except that the temperature of the polyimide film located 200 cm upstream from the pressure contact portion of the pressure roll was set to 30 ° C., and the dimensional change rate and the dimensional change rate were determined. The appearance (wavy) was evaluated. The results are shown in Table 1.
  • Example 2 A flexible copper-clad laminate was obtained by the same method as in Example 1 except that the temperature of the laminate with the protective film at a position 100 cm downstream from the pressure contact portion of the pressure roll was set to 100 ° C. The rate of change and appearance (waviness) were evaluated. The processing speed of the thermal laminating apparatus when the flexible copper-clad laminate was produced was 4 m / min. The results are shown in Table 1.

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  • Manufacturing & Machinery (AREA)
  • Physics & Mathematics (AREA)
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  • Laminated Bodies (AREA)
  • Lining Or Joining Of Plastics Or The Like (AREA)
PCT/JP2020/029687 2019-08-08 2020-08-03 積層体の製造方法 WO2021024988A1 (ja)

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WO2005063466A1 (ja) * 2003-12-26 2005-07-14 Kaneka Corporation フレキシブル積層板の製造方法
JP2005199615A (ja) * 2004-01-16 2005-07-28 Nippon Steel Chem Co Ltd 両面導体ポリイミド積層体の連続製造方法
WO2016208730A1 (ja) * 2015-06-26 2016-12-29 株式会社カネカ 片面金属張積層板の製造方法および製造装置

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JP4695421B2 (ja) 2005-03-29 2011-06-08 新日鐵化学株式会社 積層体の製造方法
JP5620093B2 (ja) * 2009-12-18 2014-11-05 株式会社カネカ 寸法安定性を向上させたフレキシブル金属張積層板の製造方法ならびにそれにより得られるフレキシブル金属張積層板
WO2016171078A1 (ja) 2015-04-23 2016-10-27 日本メクトロン株式会社 フレキシブルプリント積層板の製造装置およびフレキシブルプリント積層板の製造方法

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WO2005063466A1 (ja) * 2003-12-26 2005-07-14 Kaneka Corporation フレキシブル積層板の製造方法
JP2005199615A (ja) * 2004-01-16 2005-07-28 Nippon Steel Chem Co Ltd 両面導体ポリイミド積層体の連続製造方法
WO2016208730A1 (ja) * 2015-06-26 2016-12-29 株式会社カネカ 片面金属張積層板の製造方法および製造装置

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