WO2017051905A1 - 表面処理金属箔、積層体、プリント配線板、半導体パッケージ、電子機器及びプリント配線板の製造方法 - Google Patents

表面処理金属箔、積層体、プリント配線板、半導体パッケージ、電子機器及びプリント配線板の製造方法 Download PDF

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Publication number
WO2017051905A1
WO2017051905A1 PCT/JP2016/078117 JP2016078117W WO2017051905A1 WO 2017051905 A1 WO2017051905 A1 WO 2017051905A1 JP 2016078117 W JP2016078117 W JP 2016078117W WO 2017051905 A1 WO2017051905 A1 WO 2017051905A1
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Prior art keywords
metal foil
layer
group
resin
base material
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Ceased
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PCT/JP2016/078117
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English (en)
French (fr)
Japanese (ja)
Inventor
晃正 森山
雅史 石井
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JX Nippon Mining and Metals Corp
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JX Nippon Mining and Metals Corp
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Priority to CN201680049528.5A priority Critical patent/CN107921749A/zh
Priority to KR1020187009978A priority patent/KR20180051600A/ko
Publication of WO2017051905A1 publication Critical patent/WO2017051905A1/ja
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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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
    • B32B9/00—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00
    • 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
    • B32B9/00—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00
    • B32B9/04—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising such particular substance as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B9/041—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising such particular substance as the main or only constituent of a layer, which is next to another layer of the same or of a different material of metal
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/20—Layered products comprising a layer of metal comprising aluminium or copper
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B7/00—Layered products characterised by the relation between layers; Layered products characterised by the relative orientation of features between layers, or by the relative values of a measurable parameter between layers, i.e. products comprising layers having different physical, chemical or physicochemical properties; Layered products characterised by the interconnection of layers
    • B32B7/04—Interconnection of layers
    • B32B7/06—Interconnection of layers permitting easy separation
    • 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
    • B32B9/00—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00
    • B32B9/04—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising such particular substance as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B9/045—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising such particular substance 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
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C28/00—Coating for obtaining at least two superposed coatings either by methods not provided for in a single one of groups C23C2/00 - C23C26/00 or by combinations of methods provided for in subclasses C23C and C25C or C25D
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25D—PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
    • C25D1/00—Electroforming
    • C25D1/04—Wires; Strips; Foils
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25D—PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
    • C25D7/00—Electroplating characterised by the article coated
    • C25D7/06—Wires; Strips; Foils
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K3/00—Apparatus or processes for manufacturing printed circuits
    • H05K3/10—Apparatus or processes for manufacturing printed circuits in which conductive material is applied to the insulating support in such a manner as to form the desired conductive pattern
    • H05K3/108—Apparatus or processes for manufacturing printed circuits in which conductive material is applied to the insulating support in such a manner as to form the desired conductive pattern by semi-additive methods; masks therefor
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K3/00—Apparatus or processes for manufacturing printed circuits
    • H05K3/38—Improvement of the adhesion between the insulating substrate and the metal
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K3/00—Apparatus or processes for manufacturing printed circuits
    • H05K3/38—Improvement of the adhesion between the insulating substrate and the metal
    • H05K3/381—Improvement of the adhesion between the insulating substrate and the metal by special treatment of the substrate
    • 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
    • B32B2305/00—Condition, form or state of the layers or laminate
    • B32B2305/07—Parts immersed or impregnated in a matrix
    • B32B2305/076—Prepregs
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2307/00—Properties of the layers or laminate
    • B32B2307/70—Other properties
    • B32B2307/73—Hydrophobic
    • 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 surface-treated metal foil, a laminate, a printed wiring board, a semiconductor package, an electronic device, and a method for manufacturing a printed wiring board.
  • the following is an example of the semi-additive method using the surface profile of the latter metal foil. That is, first, the entire surface of the metal foil laminated on the resin base material is etched, the etching base material surface on which the metal foil surface profile is transferred is drilled with a laser or the like, and an electroless copper plating layer for conducting the drilled portion is formed.
  • the electroless copper plating surface is coated with a dry film, the dry film of the circuit forming part is removed by UV exposure and development, and the electroless copper plating surface not coated with the dry film is electroplated with copper.
  • the electroless copper plating layer is etched (flash etching, quick etching) with an etching solution containing sulfuric acid and hydrogen peroxide solution, and a fine circuit is formed (Patent Document 1 and Patent Document 2). ).
  • the metal foil surface profile can be transferred to the surface of the resin base material without deteriorating, and the metal foil can be removed at a good cost. There is still room for consideration.
  • the present inventors have provided a surface treatment layer such as a release layer on the surface of the metal foil so that the metal foil has a predetermined water-repellent surface.
  • a surface treatment layer such as a release layer on the surface of the metal foil so that the metal foil has a predetermined water-repellent surface.
  • a metal foil having a predetermined water-repellent surface is bonded to the resin base material and cured, and then the metal foil is removed to transfer the profile to the resin base material surface. It has been found that the layers can be laminated with good adhesion.
  • a surface-treated metal foil having a surface-treated layer on at least one surface, and a water contact angle on the surface of the surface-treated layer is 90 degrees or more. It is a surface-treated metal foil.
  • the kurtosis Rku defined by JIS B 0601 on the surface of the surface treatment layer is 2.0 to 4.0.
  • the surface treatment layer includes the release layer, and the release layer is formed by attaching the resin base material to the metal foil from the release layer side.
  • the resin base material is made peelable.
  • the release layer has the following formula: Wherein R 1 is an alkoxy group or a halogen atom, and R 2 is a hydrocarbon group selected from the group consisting of an alkyl group, a cycloalkyl group and an aryl group, or one or more hydrogen atoms are halogen atoms Any one of these hydrocarbon groups substituted by: M is any one of Al, Ti, Zr, n is 0 or 1 or 2, m is an integer from 1 to M valence, (At least one of R 1 is an alkoxy group, where m + n is a valence of M, that is, 3 for Al and 4 for Ti and Zr.)
  • the aluminate compound, the titanate compound, the zirconate compound, the hydrolysis products thereof, and the condensates of the hydrolysis products are used singly or in combination.
  • the release layer has the following formula: Wherein R 1 is an alkoxy group or a halogen atom, and R 2 is a hydrocarbon group selected from the group consisting of an alkyl group, a cycloalkyl group and an aryl group, or one or more hydrogen atoms are halogen atoms Any one of these hydrocarbon groups substituted by R 3 and R 4 are each independently a halogen atom, an alkoxy group, or a hydrocarbon group selected from the group consisting of an alkyl group, a cycloalkyl group, and an aryl group Or any one of these hydrocarbon groups in which one or more hydrogen atoms are replaced by halogen atoms.) Or a hydrolyzate thereof, or a condensate of the hydrolyzate, alone or in combination.
  • the release layer uses a compound having two or less mercapto groups in the molecule.
  • a roughened layer, a heat-resistant layer, a rust-proof layer, a chromate-treated layer, and a silane coupling-treated layer are provided between the metal foil and the release layer.
  • One or more layers selected from the group consisting of are provided.
  • the surface-treated metal foil of the present invention comprises at least one layer selected from the group consisting of the roughening treatment layer, the heat-resistant layer, the rust prevention layer, the chromate treatment layer, and the silane coupling treatment layer.
  • a resin layer is provided on the surface.
  • a resin layer is provided on the surface of the release layer side.
  • the resin layer is an adhesive resin, a primer, or a semi-cured resin.
  • the surface-treated metal foil of the present invention has a thickness of 5 to 210 ⁇ m.
  • the metal foil is a copper foil.
  • FIG. 1 Another aspect of the present invention is a laminate including the surface-treated metal foil of the present invention and a resin base material provided on the release layer side of the surface-treated metal foil.
  • the resin base material is a prepreg or contains a thermosetting resin.
  • the present invention is a printed wiring board provided with the surface-treated metal foil of the present invention.
  • the present invention is a semiconductor package provided with the printed wiring board of the present invention.
  • the present invention is an electronic device including the printed wiring board of the present invention or the semiconductor package of the present invention.
  • the surface-treated metal foil of the present invention is bonded to a resin base material from the surface-treated layer side, and the surface-treated metal foil is etched from the resin base material.
  • the circuit formed on the release surface side of the resin base material to which the surface profile is transferred is a plating pattern or a printing pattern.
  • the surface-treated metal foil of the present invention is bonded to a resin base material from the surface-treated layer side, and the surface-treated metal foil is etched from the resin base material.
  • the resin constituting the build-up layer contains a liquid crystal polymer or polytetrafluoroethylene.
  • the metal foil can be removed at a good cost without impairing the profile of the surface of the metal foil transferred to the surface of the resin substrate.
  • a buildup layer can be provided in the resin base material with favorable adhesiveness.
  • the surface-treated metal foil of the present invention is a surface-treated metal foil having a surface-treated layer on at least one surface, that is, one surface or both surfaces, and a water contact angle on the surface of the surface-treated layer is 90 degrees. That's it.
  • the surface-treated metal foil of the present invention includes a release layer, and the release layer has a resin base material bonded to the metal foil from the release layer side. The resin substrate is made peelable.
  • a surface treatment layer such as a release layer on the surface of the metal foil, the metal foil has a water-repellent surface with a water contact angle of 90 degrees or more. As a result, the metal foil is attached to the resin substrate.
  • the surface-treated metal foil has a water-repellent surface with a water contact angle of 90 degrees or more, the metal after peeling the metal foil while maintaining good peelability after bonding the metal foil and the resin base material It becomes possible to provide the resin base material surface to which the uneven profile on the foil surface is transferred and a buildup layer such as a circuit or a resin with good adhesion.
  • the water contact angle of the water repellent surface of the metal foil is preferably 90 degrees or more, and more preferably 110 degrees or more.
  • the water contact angle of the water repellent surface of the surface-treated metal foil is preferably 120 degrees or less from the viewpoint that the metal foil does not peel naturally and the peelability falls within an appropriate range.
  • the uneven shape on the surface-treated metal foil surface is also important as a factor that affects the peel strength.
  • the kurtosis Rku on the surface of the metal foil on which the release layer is provided is in the range of 2.0 to 4.0, good release properties of the metal foil and build-up of circuits and resins provided after the metal foil is peeled off It is possible to achieve both good adhesion of the layers.
  • “surface”, “surface of metal foil” and “surface of metal foil” are a roughened layer, a heat-resistant layer, a rust-proof layer, a chromate-treated layer, and a silane coupling-treated layer on the surface of the metal foil.
  • a surface treatment layer such as a release layer is provided, it means the surface after the surface treatment layer is provided (the surface of the outermost layer).
  • the release layer may be provided on both sides of the metal foil. Further, the bonding may be performed by pressure bonding. Moreover, you may provide a release layer on both surfaces of metal foil.
  • the metal foil (also referred to as raw foil) is not particularly limited, but copper foil, aluminum foil, nickel foil, copper alloy foil, nickel alloy foil, aluminum alloy foil, stainless steel foil, iron foil, iron alloy foil, etc. may be used. it can.
  • the thickness of the metal foil (raw foil) is not particularly limited, and can be, for example, 5 to 105 ⁇ m. In addition, the thickness of the metal foil is preferably 9 to 70 ⁇ m, more preferably 12 to 35 ⁇ m, and even more preferably 18 to 35 ⁇ m, since it can be easily peeled off from the resin base material. .
  • a copper foil will be described as an example of a metal foil (raw foil). Although it does not specifically limit as a manufacturing method of copper foil (raw foil), for example, an electrolytic copper foil can be produced on the following electrolysis conditions.
  • Electrolytic conditions for electrolytic green foil Cu: 30 to 190 g / L H 2 SO 4 : 100 to 400 g / L Chloride ion (Cl ⁇ ): 60 to 200 ppm by mass Nika: 1-10ppm
  • Electrolyte temperature 25-80 ° C
  • Electrolysis time 10 to 300 seconds (adjusted according to the thickness of copper to be deposited and current density)
  • Current density 50 to 150 A / dm 2
  • Electrolyte linear velocity 1.5-5m / sec
  • removing the metal foil from the resin base material means removing the metal foil from the resin base material by chemical treatment such as etching, or physically peeling the resin base material from the metal foil by peeling or the like. It means to do.
  • the resin substrate is removed after being bonded to the surface-treated metal foil of the present invention as described above, the resin substrate and the surface-treated metal foil are separated by a release layer.
  • a part of the release layer, roughened particles of the metal foil described later, a heat-resistant layer, a rust prevention layer, a chromate treatment layer, a silane coupling treatment layer, etc. may remain on the release surface of the resin base material.
  • no residue is present.
  • the surface-treated metal foil according to the present invention preferably has a peel strength of 200 gf / cm or less when the resin substrate is peeled off when the resin substrate is bonded to the metal foil from the release layer side. If controlled in this way, physical peeling of the resin base material becomes easy, and the profile on the surface of the metal foil is transferred to the resin base material better.
  • the peel strength is more preferably 150 gf / cm or less, even more preferably 100 gf / cm or less, even more preferably 50 gf / cm or less, typically 1 to 200 gf / cm, and more Typically 1 to 150 gf / cm.
  • Silane compound A silane compound having a structure represented by the following formula, a hydrolysis product thereof, or a condensate of the hydrolysis product (hereinafter simply referred to as a silane compound) is used alone or in combination.
  • R 1 is an alkoxy group or a halogen atom
  • R 2 is a hydrocarbon group selected from the group consisting of an alkyl group, a cycloalkyl group and an aryl group, or one or more hydrogen atoms are halogen atoms
  • Any one of these hydrocarbon groups substituted by R 3 and R 4 are each independently a halogen atom, an alkoxy group, or a hydrocarbon group selected from the group consisting of an alkyl group, a cycloalkyl group, and an aryl group Or any one of these hydrocarbon groups in which one or more hydrogen atoms are replaced by halogen atoms.
  • the silane compound must have at least one alkoxy group.
  • a hydrocarbon group selected from the group consisting of an alkyl group, a cycloalkyl group, and an aryl group in the absence of an alkoxy group, or any one of these hydrocarbons in which one or more hydrogen atoms are substituted with a halogen atom
  • a substituent is comprised only by group, there exists a tendency for the adhesiveness of a resin base material and metal foil to fall too much.
  • the silane compound is a hydrocarbon group selected from the group consisting of an alkyl group, a cycloalkyl group, and an aryl group, or any one of these hydrocarbon groups in which one or more hydrogen atoms are substituted with a halogen atom.
  • the alkoxy group includes an alkoxy group in which one or more hydrogen atoms are substituted with a halogen atom.
  • the silane compound has three alkoxy groups and the above hydrocarbon group (a hydrocarbon group in which one or more hydrogen atoms are substituted with a halogen atom). It is preferable to have one).
  • both R 3 and R 4 are alkoxy groups.
  • Alkoxy groups include, but are not limited to, methoxy, ethoxy, n- or iso-propoxy, n-, iso- or tert-butoxy, n-, iso- or neo-pentoxy, n-hexoxy Group, cyclohexyloxy group, n-heptoxy group, n-octoxy group and the like, straight chain, branched or cyclic carbon number of 1-20, preferably carbon number of 1-10, more preferably carbon number of 1- 5 alkoxy groups.
  • the halogen atom include a fluorine atom, a chlorine atom, a bromine atom, and an iodine atom.
  • alkyl group examples include, but are not limited to, methyl group, ethyl group, n- or iso-propyl group, n-, iso- or tert-butyl group, n-, iso- or neo-pentyl group, and n-hexyl.
  • cycloalkyl group examples include, but are not limited to, a cyclopropyl group, a cyclobutyl group, a cyclopentyl group, a cyclohexyl group, a cycloheptyl group, a cyclooctyl group, and the like, which have 3 to 10 carbon atoms, preferably 5 to 7 carbon atoms.
  • An alkyl group is mentioned.
  • the aryl group includes a phenyl group, a phenyl group substituted with an alkyl group (eg, tolyl group, xylyl group), 1- or 2-naphthyl group, anthryl group, etc., having 6 to 20, preferably 6 to 14 carbon atoms.
  • an alkyl group eg, tolyl group,
  • one or more hydrogen atoms may be substituted with a halogen atom, and may be substituted with, for example, a fluorine atom, a chlorine atom, or a bromine atom.
  • Examples of preferred silane compounds include methyltrimethoxysilane, ethyltrimethoxysilane, n- or iso-propyltrimethoxysilane, n-, iso- or tert-butyltrimethoxysilane, n-, iso- or neo-pentyl.
  • propyltrimethoxysilane, methyltriethoxysilane, hexyltrimethoxysilane, phenyltriethoxysilane, and decyltrimethoxysilane are preferable from the viewpoint of availability.
  • the silane compound in the step of forming the release layer, can be used in the form of an aqueous solution.
  • Alcohols such as methanol and ethanol can be added in order to increase the solubility in water. The addition of alcohol is particularly effective when a highly hydrophobic silane compound is used.
  • the stirring time after the silane compound is dissolved in water can be, for example, 1 to 100 hours, and typically 1 to 30 hours. Of course, there is a method of using without stirring.
  • water repellency can be improved more conventionally than by making the density
  • the concentration of the silane compound in the aqueous solution of the silane compound can be 8 to 15% by volume. When the concentration is less than 8% by volume, water repellency is insufficient (specifically, the water contact angle may be less than 90 degrees), and when it exceeds 15% by volume, poor dissolution of the silane compound occurs.
  • the first drying is performed only for the purpose of drying the aqueous solution of the silane compound.
  • the second drying has the effect of improving water repellency by terminating all condensation reactions for hydroxyl groups in the silane compound that have not undergone the condensation reaction and eliminating the remaining OH groups (hydroxyl groups).
  • the first drying can be performed at 80 to 120 ° C. ⁇ 10 seconds to 2 minutes, and the second drying can be performed at 120 to 200 ° C. ⁇ 30 seconds to 5 minutes.
  • the alcohol concentration in the solution is preferably 20 to 80% by volume in order to uniformly dissolve the silane compound that is hardly soluble in water. If the alcohol concentration in the solution is less than 20% by volume, the silane compound may not dissolve, and if it exceeds 80% by volume, the hydrolysis reaction will be incomplete. Residual, water repellency is lowered, and the contact angle of water may be reduced.
  • the pH of the aqueous solution of the silane compound is not particularly limited and can be used on either the acidic side or the alkaline side.
  • it can be used at a pH in the range of 3.0 to 10.0.
  • the pH is preferably in the range of 5.0 to 9.0, which is near neutral, and more preferably in the range of 7.0 to 9.0. .
  • the release layer is constituted by using a compound having two or more mercapto groups in the molecule, and the resin base material and the metal via the release layer. Adhesion with the foil can also be appropriately reduced to adjust the peel strength. However, when a compound having three or more mercapto groups in the molecule or a salt thereof is bonded between the resin substrate and the metal foil, it is not suitable for the purpose of reducing the peel strength.
  • Examples of the compound having two or less mercapto groups in the molecule include thiol, dithiol, thiocarboxylic acid or a salt thereof, dithiocarboxylic acid or a salt thereof, thiosulfonic acid or a salt thereof, and dithiosulfonic acid or a salt thereof. At least one selected from these can be used.
  • Thiol has one mercapto group in the molecule and is represented by, for example, R-SH.
  • R represents an aliphatic or aromatic hydrocarbon group or heterocyclic group which may contain a hydroxyl group or an amino group.
  • Dithiol has two mercapto groups in the molecule and is represented by, for example, R (SH) 2 .
  • R represents an aliphatic or aromatic hydrocarbon group or heterocyclic group which may contain a hydroxyl group or an amino group.
  • Two mercapto groups may be bonded to the same carbon, or may be bonded to different carbons or nitrogens.
  • the thiocarboxylic acid is one in which a hydroxyl group of an organic carboxylic acid is substituted with a mercapto group, and is represented by, for example, R—CO—SH.
  • R represents an aliphatic or aromatic hydrocarbon group or heterocyclic group which may contain a hydroxyl group or an amino group.
  • the thiocarboxylic acid can also be used in the form of a salt. A compound having two thiocarboxylic acid groups can also be used.
  • Dithiocarboxylic acid is one in which two oxygen atoms in the carboxy group of an organic carboxylic acid are substituted with sulfur atoms, and is represented by, for example, R- (CS) -SH.
  • R represents an aliphatic or aromatic hydrocarbon group or heterocyclic group which may contain a hydroxyl group or an amino group.
  • Dithiocarboxylic acid can also be used in the form of a salt.
  • a compound having two dithiocarboxylic acid groups can also be used.
  • the thiosulfonic acid is obtained by replacing the hydroxyl group of an organic sulfonic acid with a mercapto group, and is represented by, for example, R (SO 2 ) -SH.
  • R represents an aliphatic or aromatic hydrocarbon group or heterocyclic group which may contain a hydroxyl group or an amino group.
  • thiosulfonic acid can be used in the form of a salt.
  • Dithiosulfonic acid is one in which two hydroxyl groups of organic disulfonic acid are substituted with mercapto groups, and is represented by, for example, R-((SO 2 ) -SH) 2 .
  • R represents an aliphatic or aromatic hydrocarbon group or heterocyclic group which may contain a hydroxyl group or an amino group.
  • Two thiosulfonic acid groups may be bonded to the same carbon, or may be bonded to different carbons.
  • Dithiosulfonic acid can also be used in the form of a salt.
  • examples of the aliphatic hydrocarbon group suitable as R include an alkyl group and a cycloalkyl group, and these hydrocarbon groups may contain either or both of a hydroxyl group and an amino group.
  • alkyl group examples include, but are not limited to, methyl group, ethyl group, n- or iso-propyl group, n-, iso- or tert-butyl group, n-, iso- or neo-pentyl group, n And straight-chain or branched alkyl groups having 1 to 20, preferably 1 to 10 carbon atoms, more preferably 1 to 5 carbon atoms, such as -hexyl group, n-octyl group, and n-decyl group. .
  • cycloalkyl group is not limited, but it has 3 to 10 carbon atoms such as cyclopropyl group, cyclobutyl group, cyclopentyl group, cyclohexyl group, cycloheptyl group, cyclooctyl group, etc., preferably 5 to 7 carbon atoms.
  • cycloalkyl group preferably 3 to 10 carbon atoms.
  • suitable aromatic hydrocarbon groups as R include phenyl groups, phenyl groups substituted with alkyl groups (eg, tolyl groups, xylyl groups), 1- or 2-naphthyl groups, anthryl groups, and the like. -20, preferably 6-14 aryl groups, and these hydrocarbon groups may contain either or both of a hydroxyl group and an amino group.
  • heterocyclic group suitable as R examples include imidazole, triazole, tetrazole, benzimidazole, benzotriazole, thiazole, and benzothiazole, which may contain either or both of a hydroxyl group and an amino group.
  • Preferred examples of the compound having two or less mercapto groups in the molecule include 3-mercapto-1,2, propanediol, 2-mercaptoethanol, 1,2-ethanedithiol, 6-mercapto-1-hexanol, 1- Octanethiol, 1-dodecanethiol, 10-hydroxy-1-dodecanethiol, 10-carboxy-1-dodecanethiol, 10-amino-1-dodecanethiol, sodium 1-dodecanethiolsulfonate, thiophenol, thiobenzoic acid, Examples include 4-amino-thiophenol, p-toluenethiol, 2,4-dimethylbenzenethiol, 3-mercapto-1,2,4 triazole, and 2-mercapto-benzothiazole. Of these, 3-mercapto-1,2-propanediol is preferred from the viewpoint of water solubility and waste disposal.
  • a compound having two or less mercapto groups in the molecule can be used in the form of an aqueous solution.
  • Alcohols such as methanol and ethanol can be added in order to increase the solubility in water. The addition of alcohol is particularly effective when a compound having two or less mercapto groups in a highly hydrophobic molecule is used.
  • the peel strength can be adjusted by adjusting the concentration.
  • water repellency can be improved more conventionally than by making the density
  • the concentration of the compound having two or less mercapto groups in the molecule in the aqueous solution can be 8 to 15% by volume. When the concentration is less than 8% by volume, water repellency is insufficient (specifically, the water contact angle may be less than 90 degrees).
  • the concentration is more than 15% by volume, two or less in the molecule.
  • a compound having a mercapto group is poorly dissolved and the metal foil is laminated with a resin substrate, there is a possibility that swelling due to an unreacted compound may occur.
  • the first drying is performed only for the purpose of drying an aqueous solution of a compound having two or less mercapto groups in the molecule.
  • the second drying has the effect of improving water repellency by adjusting the arrangement of compounds having two or less mercapto groups in the molecule coordinated on the surface of the metal foil.
  • the first drying can be performed at 80 to 120 ° C. ⁇ 10 seconds to 2 minutes, and the second drying can be performed at 120 to 200 ° C. ⁇ 30 seconds to 5 minutes.
  • the alcohol concentration in the solution is a compound having 2 or less mercapto groups in the molecule which is hardly soluble in water. Is preferably 20 to 80% by volume in order to dissolve uniformly.
  • the alcohol concentration in the solution is less than 20% by volume, a compound having two or less mercapto groups in the molecule may not dissolve, and when it exceeds 80% by volume, it is densely coordinated on the surface of the metal foil. There is a possibility that the arrangement of compounds having two or less mercapto groups in the molecule is disturbed, the water repellency is lowered, and the contact angle of water is reduced.
  • the pH of the aqueous solution of the compound having two or less mercapto groups in the molecule is not particularly limited and can be used on either the acidic side or the alkaline side.
  • it can be used at a pH in the range of 3.0 to 10.0.
  • the pH is preferably in the range of 5.0 to 9.0, which is near neutral, and more preferably in the range of 7.0 to 9.0. .
  • the release layer is formed from an aluminate compound, titanate compound, zirconate compound, or a hydrolysis product thereof having a structure represented by the following formula, or a condensation product of the hydrolysis product (hereinafter simply referred to as metal alkoxide and May be used alone or in combination.
  • metal alkoxide a condensation product of the hydrolysis product
  • R 1 is an alkoxy group or a halogen atom
  • R 2 is a hydrocarbon group selected from the group consisting of an alkyl group, a cycloalkyl group and an aryl group, or one or more hydrogen atoms are halogen atoms. Any one of these substituted hydrocarbon groups, M is any one of Al, Ti, and Zr, n is 0 or 1 or 2, m is an integer from 1 to M, and R At least one of 1 is an alkoxy group.
  • M + n is the valence of M, that is, 3 for Al and 4 for Ti and Zr.
  • the metal alkoxide must have at least one alkoxy group.
  • a hydrocarbon group selected from the group consisting of an alkyl group, a cycloalkyl group, and an aryl group in the absence of an alkoxy group, or any one of these hydrocarbons in which one or more hydrogen atoms are substituted with a halogen atom
  • a substituent is comprised only by group, there exists a tendency for the adhesiveness of a resin base material and metal foil to fall too much.
  • the metal alkoxide is a hydrocarbon group selected from the group consisting of an alkyl group, a cycloalkyl group, and an aryl group, or any one of these hydrocarbon groups in which one or more hydrogen atoms are substituted with a halogen atom. It is necessary to have 0-2. This is because when there are three or more hydrocarbon groups, the adhesion between the resin base material and the metal foil tends to be too low.
  • the alkoxy group includes an alkoxy group in which one or more hydrogen atoms are substituted with a halogen atom.
  • the metal alkoxide has two or more alkoxy groups and the hydrocarbon group (a hydrocarbon in which one or more hydrogen atoms are substituted with a halogen atom). It preferably has one or two groups).
  • alkyl group examples include, but are not limited to, methyl group, ethyl group, n- or iso-propyl group, n-, iso- or tert-butyl group, n-, iso- or neo-pentyl group, n And straight-chain or branched alkyl groups having 1 to 20, preferably 1 to 10 carbon atoms, more preferably 1 to 5 carbon atoms, such as -hexyl group, n-octyl group, and n-decyl group. .
  • cycloalkyl group is not limited, but it has 3 to 10 carbon atoms such as cyclopropyl group, cyclobutyl group, cyclopentyl group, cyclohexyl group, cycloheptyl group, cyclooctyl group, etc., preferably 5 to 7 carbon atoms.
  • cycloalkyl group preferably 3 to 10 carbon atoms.
  • examples of the aromatic hydrocarbon group suitable as R 2 include a phenyl group, a phenyl group substituted with an alkyl group (eg, tolyl group, xylyl group), 1- or 2-naphthyl group, anthryl group, and the like. Examples thereof include 6 to 20, preferably 6 to 14, aryl groups, and these hydrocarbon groups may contain one or both of a hydroxyl group and an amino group.
  • one or more hydrogen atoms may be substituted with a halogen atom, and may be substituted with, for example, a fluorine atom, a chlorine atom, or a bromine atom.
  • aluminate compounds include trimethoxyaluminum, methyldimethoxyaluminum, ethyldimethoxyaluminum, n- or iso-propyldimethoxyaluminum, n-, iso- or tert-butyldimethoxyaluminum, n-, iso- or neo- Pentyl dimethoxy aluminum, hexyl dimethoxy aluminum, octyl dimethoxy aluminum, decyl dimethoxy aluminum, phenyl dimethoxy aluminum; alkyl-substituted phenyl dimethoxy aluminum (for example, p- (methyl) phenyl dimethoxy aluminum), dimethylmethoxy aluminum, triethoxy aluminum, methyl diethoxy aluminum Ethyldiethoxyaluminum, n- or iso-propyldiethyl Aluminum, n-, iso- or tert-butyldieth
  • titanate compounds examples include tetramethoxy titanium, methyl trimethoxy titanium, ethyl trimethoxy titanium, n- or iso-propyl trimethoxy titanium, n-, iso- or tert-butyl trimethoxy titanium, n-, iso- Or neo-pentyltrimethoxytitanium, hexyltrimethoxytitanium, octyltrimethoxytitanium, decyltrimethoxytitanium, phenyltrimethoxytitanium; alkyl-substituted phenyltrimethoxytitanium (eg p- (methyl) phenyltrimethoxytitanium), dimethyldimethoxy Titanium, tetraethoxy titanium, methyl triethoxy titanium, ethyl triethoxy titanium, n- or iso-propyl triethoxy titanium, n-, iso
  • zirconate compounds include tetramethoxyzirconium, methyltrimethoxyzirconium, ethyltrimethoxyzirconium, n- or iso-propyltrimethoxyzirconium, n-, iso- or tert-butyltrimethoxyzirconium, n-, iso- Or neo-pentyltrimethoxyzirconium, hexyltrimethoxyzirconium, octyltrimethoxyzirconium, decyltrimethoxyzirconium, phenyltrimethoxyzirconium; alkyl-substituted phenyltrimethoxyzirconium (eg, p- (methyl) phenyltrimethoxyzirconium), dimethyldimethoxy Zirconium, tetraethoxyzirconium, methyltriethoxyzirconium, ethyltrie
  • the metal alkoxide in the form of an aqueous solution.
  • Alcohols such as methanol and ethanol can be added in order to increase the solubility in water.
  • the addition of alcohol is particularly effective when a highly hydrophobic metal alkoxide is used.
  • the concentration of the metal alkoxide in the aqueous solution can be 8 to 15% by volume. If the concentration is less than 8% by volume, water repellency is insufficient (specifically, the water contact angle may be less than 90 degrees), and if it exceeds 15% by volume, poor dissolution of the metal alkoxide occurs. When the metal foil is laminated with the resin substrate, there is a possibility that swelling due to the unreacted compound occurs.
  • the first drying is performed only for the purpose of drying the aqueous solution of the metal alkoxide.
  • the second drying has the effect of improving the water repellency by terminating all condensation reactions for the hydroxyl groups in the metal alkoxide that have not undergone the condensation reaction and eliminating the remaining OH groups (hydroxyl groups).
  • the first drying can be performed at 80 to 120 ° C. ⁇ 10 seconds to 2 minutes, and the second drying can be performed at 120 to 200 ° C. ⁇ 30 seconds to 5 minutes.
  • the alcohol concentration in the solution is preferably 20 to 80% by volume in order to uniformly dissolve the metal alkoxide that is hardly soluble in water. If the alcohol concentration in the solution is less than 20% by volume, the metal alkoxide may not dissolve, and if it exceeds 80% by volume, the hydrolysis reaction will be incomplete, so that the metal alkoxide is not hydrolyzed as it is. Residual, water repellency is lowered, and the contact angle of water may be reduced.
  • the pH of the aqueous solution of the metal alkoxide is not particularly limited and can be used on either the acidic side or the alkaline side.
  • it can be used at a pH in the range of 3.0 to 10.0.
  • the pH is preferably in the range of 5.0 to 9.0, which is near neutral, and more preferably in the range of 7.0 to 9.0. .
  • a known release material such as a silicon-based release agent or a resin coating having a release property, can be used for the release layer.
  • the surface-treated metal foil according to the present invention is selected from the group consisting of a roughened layer, a heat-resistant layer, a rust-proof layer, a chromate-treated layer, and a silane coupling-treated layer between the metal foil and the release layer. More than one seed layer may be provided.
  • the chromate-treated layer refers to a layer treated with a liquid containing chromic anhydride, chromic acid, dichromic acid, chromate or dichromate.
  • Chromate treatment layer is any element such as cobalt, iron, nickel, molybdenum, zinc, tantalum, copper, aluminum, phosphorus, tungsten, tin, arsenic and titanium (metal, alloy, oxide, nitride, sulfide, etc.) May be included).
  • Specific examples of the chromate treatment layer include a chromate treatment layer treated with chromic anhydride or a potassium dichromate aqueous solution, a chromate treatment layer treated with a treatment solution containing anhydrous chromic acid or potassium dichromate and zinc, and the like. .
  • a roughening process layer can be formed by the following processes, for example.
  • Spherical roughening Spherical rough particles are formed using a copper roughening plating bath described below, which is made of Cu, H 2 SO 4 and As.
  • ⁇ Liquid composition 1 CuSO 4 ⁇ 5H 2 O 78 ⁇ 196g / L Cu 20-50g / L H 2 SO 4 50-200 g / L Arsenic 0.7-3.0g / L (Electroplating temperature 1) 30 ⁇ 76 °C (Current condition 1) Current density 35 to 105 A / dm 2 (above the limiting current density of the bath) (Plating time 1) 1 to 240 seconds Subsequently, plating is performed in a copper electrolytic bath made of sulfuric acid and copper sulfate in order to prevent the rough particles from falling off and to improve the peel strength.
  • the heat-resistant layer and / or the anticorrosive layer is a group of nickel, zinc, tin, cobalt, molybdenum, copper, tungsten, phosphorus, arsenic, chromium, vanadium, titanium, aluminum, gold, silver, platinum group elements, iron, tantalum
  • it may be a metal layer or an alloy layer made of one or more elements selected from the group consisting of iron, tantalum and the like.
  • the heat-resistant layer and / or rust preventive layer is a group of nickel, zinc, tin, cobalt, molybdenum, copper, tungsten, phosphorus, arsenic, chromium, vanadium, titanium, aluminum, gold, silver, platinum group elements, iron, and tantalum.
  • An oxide, nitride, or silicide containing one or more elements selected from the above may be included.
  • the heat-resistant layer and / or the rust preventive layer may be a layer containing a nickel-zinc alloy.
  • the heat-resistant layer and / or the rust preventive layer may be a nickel-zinc alloy layer.
  • the nickel-zinc alloy layer may contain 50 wt% to 99 wt% nickel and 50 wt% to 1 wt% zinc, excluding inevitable impurities.
  • the total adhesion amount of zinc and nickel in the nickel-zinc alloy layer may be 5 to 1000 mg / m 2 , preferably 10 to 500 mg / m 2 , preferably 20 to 100 mg / m 2 .
  • the amount of nickel deposited on the layer containing the nickel-zinc alloy or the nickel-zinc alloy layer is preferably 0.5 mg / m 2 to 500 mg / m 2 , and 1 mg / m 2 to 50 mg / m 2 . More preferably.
  • the heat-resistant layer and / or the rust preventive layer has a nickel or nickel alloy layer with an adhesion amount of 1 mg / m 2 to 100 mg / m 2 , preferably 5 mg / m 2 to 50 mg / m 2 , and an adhesion amount of 1 mg / m 2.
  • a tin layer of ⁇ 80 mg / m 2 , preferably 5 mg / m 2 ⁇ 40 mg / m 2 may be sequentially laminated.
  • the nickel alloy layer may be nickel-molybdenum, nickel-zinc, nickel-molybdenum-cobalt. You may be comprised by any one of these.
  • the heat-resistant layer and / or rust-preventing layer preferably has a total adhesion amount of nickel or nickel alloy and tin of 2 mg / m 2 to 150 mg / m 2 and 10 mg / m 2 to 70 mg / m 2 . It is more preferable.
  • silane coupling agent for the silane coupling agent used for a silane coupling process, for example, using an amino-type silane coupling agent or an epoxy-type silane coupling agent, a mercapto-type silane coupling agent.
  • Silane coupling agents include vinyltrimethoxysilane, vinylphenyltrimethoxylane, ⁇ -methacryloxypropyltrimethoxysilane, ⁇ -glycidoxypropyltrimethoxysilane, 4-glycidylbutyltrimethoxysilane, and ⁇ -aminopropyl.
  • Triethoxysilane N- ⁇ (aminoethyl) ⁇ -aminopropyltrimethoxysilane, N-3- (4- (3-aminopropoxy) ptoxy) propyl-3-aminopropyltrimethoxysilane, imidazolesilane, triazinesilane, ⁇ -mercaptopropyltrimethoxysilane or the like may be used.
  • the silane coupling treatment layer may be formed using a silane coupling agent such as epoxy silane, amino silane, methacryloxy silane, mercapto silane, or the like.
  • a silane coupling agent such as epoxy silane, amino silane, methacryloxy silane, mercapto silane, or the like.
  • you may use 2 or more types of such silane coupling agents in mixture.
  • it is preferable to form using an amino-type silane coupling agent or an epoxy-type silane coupling agent.
  • the amino silane coupling agent referred to here is N- (2-aminoethyl) -3-aminopropyltrimethoxysilane, 3- (N-styrylmethyl-2-aminoethylamino) propyltrimethoxysilane, 3- Aminopropyltriethoxysilane, bis (2-hydroxyethyl) -3-aminopropyltriethoxysilane, aminopropyltrimethoxysilane, N-methylaminopropyltrimethoxysilane, N-phenylaminopropyltrimethoxysilane, N- (3 -Acryloxy-2-hydroxypropyl) -3-aminopropyltriethoxysilane, 4-aminobutyltriethoxysilane, (aminoethylaminomethyl) phenethyltrimethoxysilane, N- (2-aminoethyl-3-aminopropyl
  • the silane coupling treatment layer is 0.05 mg / m 2 to 200 mg / m 2 , preferably 0.15 mg / m 2 to 20 mg / m 2 , preferably 0.3 mg / m 2 to 2.0 mg in terms of silicon atoms. / M 2 is desirable. In the case of the above-mentioned range, the adhesiveness between the resin base material and the metal foil can be further improved.
  • a resin layer may be provided on the surface of the surface-treated metal foil according to the present invention.
  • the resin layer is usually provided on the release layer.
  • the resin layer on the surface of the surface-treated metal foil may be an adhesive resin, that is, an adhesive, may be a primer, or may be a semi-cured (B-stage) insulating resin layer for adhesion. Good.
  • the semi-cured state (B stage state) is a state in which there is no sticky feeling even if the surface is touched with a finger, the insulating resin layer can be stacked and stored, and a curing reaction occurs when subjected to heat treatment. Including that.
  • the resin layer on the surface of the surface-treated metal foil is preferably a resin layer that exhibits an appropriate peel strength (for example, 2 gf / cm to 200 gf / cm) when in contact with the release layer.
  • a resin that follows the unevenness of the surface of the metal foil and hardly causes voids or bubbles that may cause blistering For example, when the resin layer is provided on the surface of the metal foil, a resin having a low viscosity such as a resin viscosity of 10,000 mPa ⁇ s (25 ° C.) or less, more preferably a resin viscosity of 5000 mPa ⁇ s (25 ° C.) or less is used. It is preferable to provide a resin layer.
  • the resin layer is the metal foil. Since it follows the surface, it is effective because it is possible to make it difficult for voids and bubbles to occur between the surface-treated metal foil and the insulating substrate.
  • the resin layer on the surface of the surface-treated metal foil may contain a thermosetting resin or a thermoplastic resin. Further, the resin layer on the surface of the surface-treated metal foil may contain a thermoplastic resin.
  • the resin layer on the surface of the surface-treated metal foil may contain a known resin, resin curing agent, compound, curing accelerator, dielectric, reaction catalyst, crosslinking agent, polymer, prepreg, skeleton material, and the like.
  • the resin layer on the surface of the surface-treated metal foil is, for example, International Publication No. WO2008 / 004399, International Publication No. WO2008 / 053878, International Publication No.
  • a laminate can be produced by providing a resin substrate on the release layer side of the surface-treated metal foil according to the present invention.
  • the resin base material is a paper base phenol resin, a paper base epoxy resin, a synthetic fiber cloth base epoxy resin, a glass cloth / paper composite base epoxy resin, a glass cloth / glass non-woven composite base epoxy resin, and You may form with glass cloth base-material epoxy resin.
  • the resin substrate may be a prepreg or may contain a thermosetting resin.
  • a printed wiring board can be produced by forming a circuit on the surface-treated metal foil of the laminate.
  • a printed circuit board can be produced by mounting electronic components on a printed wiring board.
  • the “printed wiring board” includes a printed wiring board, a printed circuit board, and a printed board on which electronic parts are mounted in this manner.
  • an electronic device may be manufactured using the printed wiring board, an electronic device may be manufactured using a printed circuit board on which the electronic components are mounted, and a print on which the electronic components are mounted.
  • An electronic device may be manufactured using a substrate.
  • the “printed circuit board” includes a circuit forming substrate for a semiconductor package.
  • a semiconductor package can be manufactured by mounting electronic components on a circuit forming substrate for a semiconductor package. Further, an electronic device may be manufactured using the semiconductor package.
  • the method for producing a printed wiring board of the present invention includes a step of bonding a resin base material from the release layer side to the surface-treated metal foil of the present invention, and the surface-treated metal foil from the resin base material.
  • a release layer is provided on the metal foil, and the resin substrate can be physically peeled when the metal foil is bonded to the resin substrate, and the metal foil is removed from the resin substrate.
  • the metal foil can be removed at a good cost without impairing the profile of the surface of the metal foil transferred to the surface of the resin base material.
  • the circuit may be formed by a plating pattern. In this case, after forming a plating pattern, a desired circuit can be formed using the plating pattern to produce a printed wiring board. Further, the circuit may be formed with a printed pattern. In this case, for example, after a print pattern is formed using an ink jet containing conductive paste or the like in the ink, a desired printed circuit is formed using the print pattern, and a printed wiring board can be manufactured.
  • a step of bonding a resin base material from the release layer side to the surface-treated metal foil of the present invention, and from the resin base material By peeling off the surface-treated metal foil without etching, a step of obtaining a resin base material in which the surface profile of the metal foil is transferred to the release surface, and the side of the release surface of the resin base material in which the surface profile is transferred Providing a build-up layer.
  • a release layer is provided on the metal foil, and the resin substrate can be physically peeled when the metal foil is bonded to the resin substrate, and the metal foil is removed from the resin substrate.
  • the metal foil can be removed at a good cost without impairing the profile of the surface of the metal foil transferred to the surface of the resin base material. Further, even if the resin component of the resin base material and the resin component of the buildup layer are different depending on the predetermined surface shape transferred to the resin base material, it is possible to bond them with good adhesion. .
  • the resin constituting the build-up layer provided on the surface of the resin base material is bonded to each other without any treatment of the resin and the resin base material (the resin constituting the build-up layer and the resin base material).
  • the strength (pull strength) when pulled and peeled off may be 500 g / cm 2 or less.
  • the “build-up layer” refers to a layer having a conductive layer, a wiring pattern or a circuit, and a resin.
  • the resin may be layered. Further, the conductive layer, the wiring pattern, or the circuit and the resin may be provided in any manner.
  • the build-up layer can be produced by providing a conductive layer, a wiring pattern or a circuit and a resin on the release surface side of the resin base material on which the surface profile of the metal foil is transferred to the release surface.
  • a method for forming the conductive layer, the wiring pattern, or the circuit a known method such as a semi-additive method, a full additive method, a subtractive method, or a partial additive method can be used.
  • the build-up layer may have a plurality of layers, or may have a plurality of conductive layers, wiring patterns or circuits and a resin (layer).
  • the plurality of conductive layers, wiring patterns, or circuits may be electrically insulated with resin.
  • the surface-treated metal foil having a release layer provided on the surface is bonded to both surfaces of the resin base material from the release layer side, and then the surface-treated metal foil is removed to form both surfaces of the resin base material.
  • a printed wiring board may be manufactured by transferring the surface profile of the surface-treated metal foil and providing a circuit, a wiring pattern, or a build-up layer on both surfaces of the resin substrate.
  • the resins, resin layers, and resin base materials described in the present specification can be used.
  • a base material or the like impregnated with a resin can be used.
  • the resin may contain an inorganic substance and / or an organic substance.
  • the resin constituting the build-up layer may be formed of a material having a low relative dielectric constant such as LCP (liquid crystal polymer) or polytetrafluoroethylene.
  • thermosetting resin such as an epoxy resin is used as a resin substrate, and it is bonded to this to provide excellent high frequency characteristics. Therefore, it is possible to provide a printed wiring board that can prevent deformation of the shape at the time of adding.
  • FIG. 1 shows a schematic example of a semi-additive method using a profile of a metal foil (for example, a copper foil).
  • a surface profile of a metal foil is used. Specifically, first, the surface-treated metal foil of the present invention is laminated on the resin base material from the release layer side to produce a laminate. Next, the metal foil of the laminate is removed by etching or peeled off. Next, after the surface of the resin base material to which the metal foil surface profile has been transferred is washed with dilute sulfuric acid or the like, electroless copper plating is performed.
  • the semi-additive method refers to a method in which a thin electroless plating is performed on a resin substrate or metal foil, a pattern is formed, and then a conductor pattern is formed using electroplating and etching. Therefore, in one embodiment of a method for producing a printed wiring board according to the present invention using a semi-additive method, a step of preparing a surface-treated metal foil and a resin base material according to the present invention, Laminating a resin base material from the release layer side on the surface-treated metal foil, After laminating the surface-treated metal foil and the resin base material, the step of removing the surface-treated metal foil by etching or peeling off, Providing a through hole or / and a blind via on the release surface of the resin base material generated by peeling off the surface-treated metal foil; Performing a desmear process on the region including the through hole or / and the blind via, Cleaning the resin substrate surface with dilute sulfuric acid for the resin substrate and the region including the through hole or / and
  • a step of preparing the surface-treated metal foil and the resin base material according to the present invention Laminating a resin base material from the release layer side on the surface-treated metal foil, After laminating the surface-treated metal foil and the resin base material, the step of removing the surface-treated metal foil by etching or peeling off, A step of washing the surface of the resin base material generated by peeling off the surface-treated metal foil, washing the surface of the resin base material with dilute sulfuric acid, and providing an electroless plating layer (for example, an electroless copper plating layer); Providing a plating resist on the electroless plating layer; Exposing the plating resist, and then removing the plating resist in a region where a circuit is formed; Providing an electrolytic plating layer (for example, an electrolytic copper plating layer) in a region where the circuit from which the plating resist has been removed is formed; Removing the plating resist;
  • an electrolytic plating layer for example, an electrolytic copper plating layer
  • a circuit is formed on the release surface of the resin base material after the surface-treated metal foil is peeled off, and a printed circuit formation substrate and a circuit formation substrate for a semiconductor package can be manufactured. Furthermore, a printed wiring board and a semiconductor package can be manufactured using the circuit formation substrate. Furthermore, an electronic device can be manufactured using the printed wiring board and the semiconductor package.
  • a step of preparing the surface-treated metal foil and the resin base material according to the present invention Laminating a resin base material from the release layer side on the surface-treated metal foil, After laminating the surface-treated metal foil and the resin base material, the step of removing the surface-treated metal foil by etching or peeling off, The step of washing the resin substrate surface with dilute sulfuric acid or the like for the release surface of the resin substrate produced by peeling off the surface-treated metal foil, Providing a plating resist on the cleaned resin substrate surface; Exposing the plating resist, and then removing the plating resist in a region where a circuit is formed; Providing an electroless plating layer (for example, an electroless copper plating layer or a thick electroless plating layer) in a region where the circuit from which the plating resist has been removed is formed; Removing the plating resist; including.
  • an electroless plating layer for example, an electroless copper plating layer or a thick electroless plating layer
  • the electroless plating layer can be easily provided by cleaning the surface of the resin base material.
  • a part or all of the release layer is removed from the surface of the resin base material by the cleaning.
  • cleaning by a known cleaning method (type of liquid to be used, temperature, liquid application method, etc.) can be used. Further, it is preferable to use a cleaning method capable of removing a part or all of the release layer of the present invention.
  • a circuit is formed on the release surface of the resin base material after the surface-treated metal foil is peeled off, and a printed circuit forming substrate and a circuit forming substrate for a semiconductor package can be manufactured. Furthermore, a printed wiring board and a semiconductor package can be manufactured using the circuit formation substrate. Furthermore, an electronic device can be manufactured using the printed wiring board and the semiconductor package.
  • the surface of the surface-treated metal foil was measured with a scanning electron microscope or the like equipped with XPS (X-ray photoelectron spectrometer), EPMA (electron beam microanalyzer), EDX (energy dispersive X-ray analysis), and Si was If detected, it can be inferred that a silane compound is present on the surface of the surface-treated metal foil. Further, when the peel strength (peel strength) between the surface-treated metal foil and the resin substrate is 200 gf / cm or less, it can be estimated that the silane compound that can be used for the release layer of the present invention is used. .
  • the surface of the surface-treated metal foil is measured with an apparatus such as a scanning electron microscope equipped with XPS (X-ray photoelectron spectrometer), EPMA (electron beam microanalyzer), EDX (energy dispersive X-ray analysis), and S is
  • XPS X-ray photoelectron spectrometer
  • EPMA electron beam microanalyzer
  • EDX energy dispersive X-ray analysis
  • the surface of the surface-treated metal foil is measured with a scanning electron microscope equipped with XPS (X-ray photoelectron spectrometer), EPMA (electron beam microanalyzer), EDX (energy dispersive X-ray analysis), Al,
  • XPS X-ray photoelectron spectrometer
  • EPMA electron beam microanalyzer
  • EDX energy dispersive X-ray analysis
  • Al aluminum
  • Roughening Spherical roughening
  • Spherical roughened particles were formed using a copper roughening plating bath described below consisting of Cu, H 2 SO 4 and As.
  • ⁇ Liquid composition 1 CuSO 4 ⁇ 5H 2 O 78 ⁇ 118g / L Cu 20-30g / L H 2 SO 4 12g / L Arsenic 1.0-3.0g / L (Electroplating temperature 1) 25-33 ° C (Current condition 1) Current density 78 A / dm 2 (above the limiting current density of the bath) (Plating time 1) 1 to 45 seconds
  • plating was performed in a copper electrolytic bath made of sulfuric acid and copper sulfate in order to prevent falling off of the roughened particles and to improve the peel strength.
  • release layer A A water-methanol mixed solution containing a silane compound (n-propyltrimethoxysilane) in a volume ratio of 8 vol% is applied to the treated surface of the metal foil (copper foil) using a spray coater, and then air at 100 ° C. Then, the surface of the copper foil was dried for 1 minute, followed by heat treatment in air at 150 ° C. for 1 minute to form a release layer A.
  • the stirring time from dissolving the silane compound in water to before coating was 30 hours, the methanol concentration in the solution was 40 vol% by volume, and the pH of the aqueous solution was 3.8 to 4.2.
  • [Release layer B] A water-methanol mixed solution containing a silane compound (n-hexyltrimethoxysilane) in a volume ratio of 8 vol% is applied to the treated surface of the metal foil (copper foil) using a spray coater, and then air at 100 ° C. Then, the surface of the copper foil was dried for 1 minute, followed by heat treatment in air at 150 ° C. for 1 minute to form a release layer B.
  • the stirring time from dissolving the silane compound in water to before coating was 30 hours, the methanol concentration in the solution was 40 vol% by volume, and the pH of the aqueous solution was 3.8 to 4.2.
  • [Release layer C] A water-methanol mixed solution containing a silane compound (n-decyltrimethoxysilane) in a volume ratio of 8 vol% is applied to the treated surface of the metal foil (copper foil) using a spray coater, and then air at 100 ° C. Then, the surface of the copper foil was dried for 1 minute, followed by heat treatment in air at 150 ° C. for 1 minute to form a release layer C. The stirring time from dissolving the silane compound in water to before coating was 30 hours, the methanol concentration in the solution was 40 vol% by volume, and the pH of the aqueous solution was 3.8 to 4.2.
  • a silane compound n-decyltrimethoxysilane
  • [Release layer D] A water-methanol mixed solution containing a silane compound (dimethyldimethoxysilane) in a volume ratio of 8 vol% is applied to the treated surface of the metal foil (copper foil) using a spray coater, and then 1 in 100 ° C. air. After the copper foil surface was dried for 1 minute, a heat treatment was performed in air at 150 ° C. for 1 minute to form a release layer B. The stirring time from dissolving the silane compound in water to before coating was 30 hours, the methanol concentration in the solution was 40 vol% by volume, and the pH of the aqueous solution was 3.8 to 4.2.
  • a silane compound dimethyldimethoxysilane
  • [Release layer E] A water-methanol mixed solution containing a silane compound (trifluoropropyltrimethoxysilane) in a volume ratio of 8 vol% is applied to the treated surface of the metal foil (copper foil) using a spray coater, and then air at 100 ° C. Then, the surface of the copper foil was dried for 1 minute, followed by heat treatment in air at 150 ° C. for 1 minute to form a release layer B. The stirring time from dissolving the silane compound in water to before coating was 30 hours, the methanol concentration in the solution was 40 vol% by volume, and the pH of the aqueous solution was 3.8 to 4.2.
  • a silane compound trifluoropropyltrimethoxysilane
  • [Release layer F] Sodium 1-dodecanethiolsulfonate is used as a compound having two or less mercapto groups in the molecule, and a water-methanol mixed solution of sodium 1-dodecanethiolsulfonate (sodium 1-dodecanethiolsulfonate: 8 vol%) is used. After applying to the treated surface of the metal foil (copper foil) using a spray coater, the copper foil surface was dried in air at 100 ° C. for 1 minute and then heat-treated in air at 150 ° C. for 1 minute. A release layer F was formed. The methanol concentration in the solution was 40 vol% by volume, and the pH of the solution was 5-9.
  • Triisopropoxyaluminum which is an aluminate compound, is used as the metal alkoxide, and a water-methanol mixed solution of triisopropoxyaluminum (triisopropoxyaluminum concentration: 8 vol%) is treated with a spray coater on the metal foil (copper foil). After coating on the surface, the surface of the copper foil was dried in air at 100 ° C. for 1 minute, and then heat-treated in air at 150 ° C. for 1 minute to form a release layer G. The stirring time from when the aluminate compound was dissolved in water to before coating was 2 hours, the alcohol concentration in the solution was 40 vol% by volume, and the pH of the solution was 5-9.
  • Example 1 Resin layer formation treatment
  • a resin layer was further formed under the following conditions.
  • Resin synthesis example To a 2-liter three-necked flask equipped with a stainless steel vertical stirring bar, a trap with a nitrogen inlet tube and a stopcock, and a reflux condenser with a ball condenser, 117.68 g (400 mmol) of 4′-biphenyltetracarboxylic dianhydride, 87.7 g (300 mmol) of 1,3-bis (3-aminophenoxy) benzene, 4.0 g (40 mmol) of ⁇ -valerolactone, 4.
  • NMP N-methyl-2-pyrrolidone
  • toluene 20 g 8 g (60 mmol), N-methyl-2-pyrrolidone (hereinafter referred to as NMP) 300 g, and toluene 20 g were added, heated at 180 ° C. for 1 hour, cooled to near room temperature, and then 3, 4, 3 ′, 4′- 29.42 g (100 mmol) of biphenyltetracarboxylic dianhydride, 82.12 g of 2,2-bis ⁇ 4- (4-aminophenoxy) phenyl ⁇ propane (200 mmol), 200 g of NMP, and 40 g of toluene were added, mixed at room temperature for 1 hour, and then heated at 180 ° C.
  • NMP N-methyl-2-pyrrolidone
  • the block copolymerized polyimide solution obtained in the synthesis example was further diluted with NMP to obtain a block copolymerized polyimide solution having a solid content of 10%.
  • bis (4-maleimidophenyl) methane BMI-H, Kay-Isei
  • Bis (4-maleimidophenyl) methane solid content weight: block copolymerized polyimide solid content weight contained in resin solution 35: 65
  • a resin solution was prepared by dissolving and mixing at 60 ° C. for 20 minutes.
  • the resin solution is coated on the release layer forming surface, dried in a nitrogen atmosphere at 120 ° C. for 3 minutes, and at 160 ° C. for 3 minutes, and finally heat-treated at 300 ° C. for 2 minutes to obtain a resin layer.
  • the copper foil provided with was produced.
  • the thickness of the resin layer was 2 ⁇ m.
  • Kurtosis (Rku) Kurtosis (Rku) on the surface of the metal foil was measured in a JIS B 0601 2001 compliant mode using a laser microscope OLS4100 manufactured by Olympus Corporation. The measurement length was 258 ⁇ m. The temperature during measurement was 23 to 25 ° C.
  • a resin layer composed of a liquid crystal polymer (assuming a resin constituting the build-up layer) was laminated on the release surface of the resin substrate after peeling (Example 3).
  • a reliability test (heating test at 250 ° C. ⁇ 10 ° C. ⁇ 1 hour).
  • the size of the evaluation sample was 250 mm ⁇ 250 mm, and three samples were measured for each sample number. The case where circuit peeling and substrate swelling did not occur was evaluated as “ ⁇ ”. Slight circuit peeling or substrate swelling occurred (3 or less in one sample), but those that could be used as a product when the locations to be used were selected were evaluated as “ ⁇ ”.
  • a large number of circuit peeling or substrate swelling occurred (more than 3 in one sample), and those that could not be used as a product were evaluated as “x”.
  • Table 1 shows the test conditions and evaluation results.
  • the water contact angle on the surface of the surface treatment layer is 90 degrees or more, and the peelability when physically peeling the metal foil from the resin base material is good. The occurrence of swelling was successfully suppressed.
  • the water contact angle on the surface of the surface treatment layer side is less than 90 degrees, the peelability when physically peeling the metal foil from the resin base material is poor, and circuit peeling and generation of substrate swelling are caused. It was not possible to suppress well.

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  • Chemical Kinetics & Catalysis (AREA)
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  • Laminated Bodies (AREA)
  • Manufacturing Of Printed Wiring (AREA)
  • Electroplating Methods And Accessories (AREA)
  • Other Surface Treatments For Metallic Materials (AREA)
PCT/JP2016/078117 2015-09-25 2016-09-23 表面処理金属箔、積層体、プリント配線板、半導体パッケージ、電子機器及びプリント配線板の製造方法 Ceased WO2017051905A1 (ja)

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US10581081B1 (en) * 2019-02-01 2020-03-03 Chang Chun Petrochemical Co., Ltd. Copper foil for negative electrode current collector of lithium ion secondary battery
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