US20100215982A1 - Metal Covered Polyimide Composite, Process for Producing the Composite, and Apparatus for Producing the Composite - Google Patents

Metal Covered Polyimide Composite, Process for Producing the Composite, and Apparatus for Producing the Composite Download PDF

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Publication number
US20100215982A1
US20100215982A1 US12/738,095 US73809508A US2010215982A1 US 20100215982 A1 US20100215982 A1 US 20100215982A1 US 73809508 A US73809508 A US 73809508A US 2010215982 A1 US2010215982 A1 US 2010215982A1
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Prior art keywords
layer
copper
plating
zone
producing
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Michiya Kohiki
Naonori Michishita
Nobuhito Makino
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JX Nippon Mining and Metals Corp
Nippon Mining Holdings Inc
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Nippon Mining and Metals Co Ltd
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Assigned to NIPPON MINING & METALS CO., LTD. reassignment NIPPON MINING & METALS CO., LTD. ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: MAKINO, NOBUHITO, MICHISHITA, NAONORI, KOHIKI, MICHIYA
Publication of US20100215982A1 publication Critical patent/US20100215982A1/en
Assigned to NIPPON MINING HOLDINGS, INC. reassignment NIPPON MINING HOLDINGS, INC. MERGER (SEE DOCUMENT FOR DETAILS). Assignors: NIPPON MINING & METALS CO., LTD.
Assigned to JX NIPPON MINING & METALS CORPORATION reassignment JX NIPPON MINING & METALS CORPORATION CHANGE OF NAME (SEE DOCUMENT FOR DETAILS). Assignors: NIPPON MINING HOLDINGS, INC.
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    • 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
    • C23C28/02—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 only coatings only including layers of metallic material
    • C23C28/023—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 only coatings only including layers of metallic material only coatings of metal elements only
    • 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
    • C23C18/00—Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating
    • C23C18/16—Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating by reduction or substitution, e.g. electroless plating
    • C23C18/1601—Process or apparatus
    • 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
    • C23C18/00—Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating
    • C23C18/16—Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating by reduction or substitution, e.g. electroless plating
    • C23C18/1601—Process or apparatus
    • C23C18/1633—Process of electroless plating
    • C23C18/1646—Characteristics of the product obtained
    • C23C18/165—Multilayered product
    • C23C18/1653—Two or more layers with at least one layer obtained by electroless plating and one layer obtained by electroplating
    • 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
    • C23C28/02—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 only coatings only including layers of metallic material
    • C23C28/021—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 only coatings only including layers of metallic material including at least one metal alloy layer
    • 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
    • C23C28/02—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 only coatings only including layers of metallic material
    • C23C28/028—Including graded layers in composition or in physical properties, e.g. density, porosity, grain size
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25D—PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
    • C25D5/00—Electroplating characterised by the process; Pretreatment or after-treatment of workpieces
    • C25D5/10—Electroplating with more than one layer of the same or of different metals
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25D—PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
    • C25D5/00—Electroplating characterised by the process; Pretreatment or after-treatment of workpieces
    • C25D5/60—Electroplating characterised by the structure or texture of the layers
    • C25D5/615—Microstructure of the layers, e.g. mixed structure
    • C25D5/617—Crystalline layers
    • 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
    • C25D7/0614—Strips or foils
    • C25D7/0635—In radial cells
    • 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
    • H05K3/22—Secondary treatment of printed circuits
    • H05K3/24—Reinforcing the conductive pattern
    • H05K3/241—Reinforcing the conductive pattern characterised by the electroplating method; means therefor, e.g. baths or apparatus
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0313—Organic insulating material
    • H05K1/032—Organic insulating material consisting of one material
    • H05K1/0346—Organic insulating material consisting of one material containing N
    • 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
    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/01—Dielectrics
    • H05K2201/0137—Materials
    • H05K2201/0154—Polyimide
    • 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
    • H05K2203/00—Indexing scheme relating to apparatus or processes for manufacturing printed circuits covered by H05K3/00
    • H05K2203/14—Related to the order of processing steps
    • H05K2203/1476—Same or similar kind of process performed in phases, e.g. coarse patterning followed by fine patterning
    • 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
    • H05K2203/00—Indexing scheme relating to apparatus or processes for manufacturing printed circuits covered by H05K3/00
    • H05K2203/15—Position of the PCB during processing
    • H05K2203/1545—Continuous processing, i.e. involving rolls moving a band-like or solid carrier along a continuous production path
    • 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
    • H05K3/02—Apparatus or processes for manufacturing printed circuits in which the conductive material is applied to the surface of the insulating support and is thereafter removed from such areas of the surface which are not intended for current conducting or shielding
    • H05K3/022—Processes for manufacturing precursors of printed circuits, i.e. copper-clad substrates
    • 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
    • H05K3/388—Improvement of the adhesion between the insulating substrate and the metal by the use of a metallic or inorganic thin film adhesion layer
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/12—All metal or with adjacent metals
    • Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
    • Y10T428/12771—Transition metal-base component
    • Y10T428/12806—Refractory [Group IVB, VB, or VIB] metal-base component
    • Y10T428/12826—Group VIB metal-base component
    • Y10T428/12847—Cr-base component
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/12—All metal or with adjacent metals
    • Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
    • Y10T428/12771—Transition metal-base component
    • Y10T428/12861—Group VIII or IB metal-base component
    • Y10T428/12903—Cu-base component
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/12—All metal or with adjacent metals
    • Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
    • Y10T428/12771—Transition metal-base component
    • Y10T428/12861—Group VIII or IB metal-base component
    • Y10T428/12903—Cu-base component
    • Y10T428/1291—Next to Co-, Cu-, or Ni-base component

Definitions

  • the present invention relates to a metal covered polyimide composite for use as a mounting material of electronic components such as a flexible print substrate, TAB, COF (Chip on Film), and additionally relates to a method of producing the composite and an apparatus for producing the composite.
  • FCCL Flexible Copper Clad Laminate
  • metal conductor layers primarily formed from copper are laminated on a polyimide film
  • FCCL Flexible Copper Clad Laminate
  • a non-adhesive flexible laminate especially a two-layer flexible laminate that does not include an adhesive layer between a polyimide film and a metal layer is catching attention on the demands of finer pitches of the circuit wiring width.
  • a method of producing a non-adhesive flexible laminate in particular a non-adhesive flexible laminate capable of accommodating fine pitches, primarily performed is a so-called metalizing method of forming, in advance, a tie-coat layer configured from a material having favorable adhesion with polyimide on a polyimide film by a drying method such as sputtering, CVD, or vapor deposition and a metal seed layer as a conductor of the cathode/current in the subsequent electroplating process, and thereafter forming a metal layer film to become the conductor layer of the circuit board by way of electroplating (refer to Patent Literature 1).
  • modification is carried out by performing plasma treatment to the polyimide film surface in order to eliminate the contaminants on the surface and to improve the surface roughness prior to forming the metal layer (refer to Patent Literature 2 and Patent Literature 3).
  • a polyimide film with a metal film for use in TAB or FPC obtained by performing chemical etching to the polyimide film surface so to roughen the surface, forming a foundation layer thereon, and additionally forming a copper vapor deposition layer thereon (refer to Patent Literature 5).
  • a metal covered polyimide composite When a metal covered polyimide composite is to be used as a mounting material of electronic components such as a COF (Chip on Film), the metal layer on the polyimide is partially eliminated to create a circuit pattern, tin plating is subsequently performed on the copper layer forming the circuit pattern, and treatment such as solder resist or resin seal is additionally performed on the tin plated layer.
  • tin plating is subsequently performed on the copper layer forming the circuit pattern
  • treatment such as solder resist or resin seal is additionally performed on the tin plated layer.
  • a major cause of such peeling is the Kirkendall voids (air gaps) that are generated between the copper layer and the tin plated layer due to the electroplating process.
  • the Kirkendall voids will be explained in detail later.
  • An electroplated copper layer is usually formed with a plurality of electrolytic baths, and the electroplating current conditions of the copper layer will change considerably among the electrolytic baths as a matter of course.
  • the portions in which the electroplating current conditions change considerably will become boundaries in the copper plated layer since the intake of copper crystal grains, impurities and the like will differ from the other portions. Since the Kirkendall voids particularly occur at the portions where the copper plated layer boundary and the tin plated layer are adjacent to each other, if plating is to be performed in multiple electroplating baths, then the Kirkendall voids will arise at least in a quantity that is equivalent to the number of electroplating baths.
  • Patent Literature 6 has analyzed that the Kirkendall voids causes the peeling.
  • Patent Literature 6 only sees the tin covered on the uppermost layer of the copper plating as the problem.
  • the tin layer will cover the side face in addition to the uppermost layer of the copper.
  • the foregoing method is a sufficient solution to the problem.
  • the drum electroplating method is a method of feeding a polyimide film, in which a tie-coat layer and a metal seed layer are formed thereon by electroless plating or a drying method, around a drum surface that is dipped in an electrolyzer, and thereby performing copper plating to the surface.
  • this method is able to move the anode and cathode closer without disturbances such as the warping or blurring during the feeding of the film to become the cathode and to control the distance constant between the anode and cathode, it is possible to increase the current density. Moreover, as a result of moving the anode and cathode closer together, the flow velocity of the plating electrolytic solution can also be increased easily, and this is also effective in increasing the current density. Accordingly, the drum electroplating method is effective in decreasing the Kirkendall voids.
  • this drum electroplating method also entails its own problems. It is necessary to increase the current density in order to increase the electrodeposition rate of the electroplating process.
  • the metal seed layer formed on the polyimide surface is unable to withstand a large current since its thickness is limited. Consequently, the anodes that set to face the drum are divided into a plurality of zones (plating zones), and the current density to the respective zones is being controlled independently.
  • an object of the present invention is to provide a metal covered polyimide composite which can effectively prevent peeling in a non-adhesive flexible laminate (especially a two-layer flexible laminate), and particularly can effectively inhibit peeling from the interface of a copper layer and a tin plating, as well as provide a method of producing the composite and an apparatus for producing the composite.
  • the present invention provides:
  • a metal covered polyimide composite comprising a tie-coat layer and a metal seed layer formed on a surface of a polyimide film by electroless plating or a drying method, and a copper layer or a copper alloy layer formed thereon by electroplating, wherein the copper plated layer or copper alloy plated layer includes three layers to one layer of the copper layer or copper alloy layer;
  • the present invention additionally provides:
  • a method of producing a metal covered polyimide composite wherein a tie-coat layer and a metal seed layer on a surface of a polyimide film by electroless plating or a drying method, three layers to one layer of an electroplated layer of copper or copper alloy are additionally formed thereon;
  • the present invention further provides:
  • An apparatus for producing a metal covered polyimide composite comprising an electroplating bath, a plating drum in which a part thereof is dipped in the electroplating bath, a unit for feeding a polyimide film to be plated, in which a tie-coat layer and a metal seed layer are formed on its surface by electroless plating or a drying method, around the plating drum, and a unit for supplying current to the plated surface of the polyimide film with the tie-coat layer and metal seed layer formed thereon, wherein one or more anodes are set to face the drum, and the plating zone is divided into one to four zones;
  • a metal covered polyimide composite, a method of producing the composite and an apparatus for producing the composite of the present invention can effectively prevent peeling in a non-adhesive flexible laminate (especially a two-layer flexible laminate), particularly can effectively inhibit peeling from the interface of a copper layer and a tin plating, and yield a superior effect of being able to improve the adhesion strength.
  • FIG. 1 [ FIG. 1 ]
  • FIG. 2 [ FIG. 2 ]
  • FIG. 3 [ FIG. 3 ]
  • FIG. 5 [ FIG. 5 ]
  • the present invention includes cases of copper alloy plating in addition to copper plating, but in order to simplify the explanation these will be collectively explained as copper plating.
  • the basic process is to form a metal layer on at least one face of the polyimide film by the sputtering method, and additionally form a metal conductor layer formed from a copper layer or copper alloy layer on the foregoing surface in order to prepare a non-adhesive flexible laminate.
  • the polyimide film surface is subject to plasma treatment in order to eliminate the contaminants on the surface and modify the surface.
  • a sputtered metal layer (so-called tie-coat layer) of 5 to 300 nm is formed on the surface of the polyimide film.
  • the sputtered metal layer is selected from one type among nickel, chromium, cobalt, nickel alloy, chromium alloy, and cobalt alloy.
  • a polyimide film having a thickness of 12.5 ⁇ m to 50 ⁇ m can be used, but this thickness is required to the circuit board, and there is no particular limitation regarding the thickness.
  • Upilex by Ube Industries, Kapton by DuPont-Toray, Apical by Kaneka or the like is used, but there is also no particular limitation regarding the type of polyimide film to be used.
  • the tie-coat layer has the function of increasing the adhesive strength between the metal layer and the polyimide [film], and increasing the stability under a heat-resistant and moisture-resistant environment.
  • a copper layer of 150 to 500 nm to become the metal seed layer is formed on the tie-coat layer by sputtering.
  • the sputtered copper layer will become the conductor of the cathode/current in the subsequent electroplating process.
  • an electroplated layer formed from copper or copper alloy is formed on the metal seed layer.
  • the electroplating apparatus shown in FIG. 1 is used as the plating system.
  • This electroplating apparatus comprises an electroplating bath, a plating drum in which a part thereof (approximately half) is dipped in the electroplating bath, a unit for feeding a polyimide film plated around the plating drum, a unit for supplying current to the plated surface of the polyimide film, and one or more anodes facing the drum.
  • these anodes are so-called insoluble anodes, and the supply of copper ions for copper plating is performed by supplying an electrolytic solution, in which copper is separately dissolved and in which the copper concentration is adjusted, to the electrolytic bath.
  • the copper or copper alloy plating system that is used in the present invention is a one or two bath-type plating system.
  • Cell A a bath
  • Cell B the other bath
  • the one bath-type plating system only has Cell A.
  • Anodes are set to face the drum for each of these zones.
  • the solution sending method where the electroplating solution is supplied from the lower part of the electroplating bath and overflows from the upper part of the electroplating bath is adopted. This supply method is able to control the flow velocity and is necessary to form a uniform plated layer. Moreover, the current of each anode zone can be adjusted independently.
  • a plating method of arranging numerous plating baths in parallel and repeatedly dipping a continuously wound polyimide film in a plating bath was adopted.
  • a copper plated layer was conventionally formed according to the foregoing method. Based on this method, since there is no limit in the number of plating baths, plating can be performed to multiple layers as many as plating baths.
  • the copper layer of the metal covered polyimide composite obtained as described above is etched with an etching solution to form a conductive circuit. Then, tin plating is formed on the copper circuit and solder resist, resin or the like is used additionally to cover the same. In the foregoing case, peeling between the copper circuit layer and tin plated layer and cracks in the tin layer will become a problem.
  • the Kirkendall voids do not arise easily at room temperature, diffusion will advance due to the foregoing mechanism, and the Kirkendall voids are generated thereby during the heat treatment at roughly 80 to 150° C. after the tin plating, and the heat treatment at roughly 150 to 160° C. in the processes of solder resist, resin seal and the like.
  • the foregoing heat treatment processes are indispensible in producing wiring boards, and it can be said that this is an unavoidable problem so as long as discontinuous portions of the interface exists.
  • the drum-based two-bath copper plating system if a once-plated surface is exposed to the atmosphere and additionally plated again, a copper layer boundary (discontinuous layer) will be formed.
  • a drum-based two-bath plating system it is difficult to completely inhibit the Kirkendall voids.
  • the present invention provides an apparatus for producing a metal covered polyimide composite in a drum plating system comprising an electroplating bath, a plating drum in which a part thereof (approximately half) is dipped in the electroplating bath, a unit for feeding a polyimide film to be plated around the plating drum, a unit for supplying current to the plated surface of the polyimide film, and one or more anodes facing the drum, wherein the plating zone is divided into three zones to one zone, and the copper layer or copper alloy layer is formed as three layers to one layer.
  • the present invention additionally provides a method and apparatus for producing a metal covered polyimide composite in which the number of boundaries between the respective copper layers or copper alloy layers is two to zero.
  • the distance L between zone 3 and zone 4 (or distance L between zone 7 and zone 8) is adjusted to be preferably double or less than the distance d between the anode and the plating object, and more preferably 1 ⁇ 2 or less.
  • the number of copper or copper alloy electroplating baths is few as possible, which is because an unavoidable discontinuous interface will occur as described.
  • the use of one or two baths would be a desirable condition.
  • the material used as the polyimide film there is no particular limitation in the material used as the polyimide film.
  • Upilex by Ube Industries, Kapton by DuPont-Toray, Apical by Kaneka are commercially available, and any one of these polyimide films can be applied in the present invention.
  • the present invention is not limited to this kind of specific variety.
  • Upilex-SGA by Ube Industries is used as the polyimide film.
  • the polyimide film was placed in a vacuum apparatus and, after evacuation, the polyimide film was subject to surface modification treatment using plasma.
  • a tie-coat layer (Ni-20 wt % Cr) of 25 nm was formed on the foregoing polyimide film surface subject to the plasma treatment by way of sputtering.
  • a metal seed layer (copper layer) of 300 nm was formed by sputtering.
  • the drum-based two bath-type electroplating apparatus shown in FIG. 1 was used to form a metal conductor layer (total thickness of approximately 8 ⁇ m) formed of copper on the surface of the foregoing metal seed layer by way of electroplating using a copper sulfate plating bath, whereby a two-layer flexible laminate was prepared.
  • a metal conductor layer total thickness of approximately 8 ⁇ m
  • the anodes in zone 3 and zone 4 were electrically connected, and the distance L between zone 3 and zone 4 was adjusted to be approximately 1 ⁇ 2 of the distance d between the anode and the plating object in order to form the copper plated layer.
  • a copper plated layer of 3.90 ⁇ m was formed in zone 3+zone 4, that of 2.07 ⁇ m in zone 7, and that of 2.20 ⁇ m in zone 8.
  • a copper plated layer of 0.05 ⁇ m was formed in zone 1, that of 0.27 ⁇ m in zone 2, and that of 0 ⁇ m in zone 5 and zone 6, respectively.
  • FIG. 2 is a result of performing chemical polishing of dipping the copper layer for 15 seconds in an aqueous solution of NH 3 :29%, H 2 O 2 :1%.
  • zone 3+zone 4 the thickness of the copper layer was approximately two zones' worth, and the thickness of the copper layers formed in other zone 7+zone 8 has hardly any difference, so it is evident that a uniform layer was formed.
  • this copper layer was etched to form a circuit, and a tin plated layer of approximately 0.3 ⁇ m was additionally formed on the copper circuit by dipping it into a tin plating bath of AT-501 manufactured by Nikko Mining & Metals at 50° C. for 3 minutes.
  • the copper layer was annealed at 120° C. ⁇ 12 hours, and the cross section was observed. This cross section is similarly a result of performing chemical polishing of dipping the copper layer for 15 seconds in an aqueous solution of NH 3 :29%, H 2 O 2 :1%. The results are shown in FIG. 3 .
  • the drum-based two bath-type electroplating apparatus shown in FIG. 1 was used to form the copper plated layer wherein, in order to reduce the number of zones, in Cell A, zone 3 and zone 4 were electrically connected, and the distance L between zone 3 and zone 4 was adjusted to be approximately 1 ⁇ 2 of the distance d between the anode and the plating object in order to form the copper plated layer; and, in Cell B, zone 7 and zone 8 were electrically connected, and the distance L between zone 7 and zone 8 was adjusted to be approximately 1 ⁇ 2 of the distance d between the anode and the plating object.
  • a copper plated layer of 0.05 ⁇ m was formed in zone 1, that of 0.27 ⁇ m in zone 2, and that of 0 ⁇ m in zone 5 and zone 6, respectively.
  • FIG. 4 is a result of performing chemical polishing of dipping the copper layer for 15 seconds in an aqueous solution of NH 3 :29%, H 2 O 2 :1%.
  • zone 3+zone 4 the thickness of the copper layer was approximately two zones' worth, and so was the thickness of the copper layers formed in other zone 7+zone 8, but the thickness of the copper layers has hardly any difference, so it is evident that a uniform layer was formed.
  • this copper layer was etched to form a circuit, and a tin plated layer of approximately 0.3 ⁇ m was additionally formed on the copper circuit by dipping it into a tin plating bath of AT-501 manufactured by Nikko Mining & Metals at 50° C. for 3 minutes.
  • the copper layer was annealed at 120° C. ⁇ 12 hours, and the cross section was observed. This cross section is similarly a result of performing chemical polishing of dipping the copper layer for 15 seconds in an aqueous solution of NH 3 :29%, H 2 O 2 :1%.
  • the copper plated layer was formed upon turning off the current of zone 1 and zone 2.
  • dummy anodes prepared with an insulating material in the same shape was disposed in place of the normal anodes in zone 1 and zone 2.
  • zone 1 and zone 2 were 0 ⁇ m in zone 1 and zone 2 and 0 ⁇ m in zone 5 and zone 6.
  • FIG. 6 is a result of performing chemical polishing of dipping the copper layer for 15 seconds in an aqueous solution of NH 3 :29%, H 2 O 2 :1%.
  • zone 3+zone 4 the thickness of the copper layer was approximately two zones' worth, and so was the thickness of the copper layers formed in other zone 7+zone 8, but the thickness of the copper layers has hardly any difference, so it is evident that a uniform layer was formed.
  • this copper layer was etched to form a circuit, and a tin plated layer of approximately 0.3 ⁇ m was additionally formed on the copper circuit by dipping it into a tin plating bath of AT-501 manufactured by Nikko Mining & Metals at 50° C. for 3 minutes.
  • the copper layer was annealed at 120° C. ⁇ 12 hours, and the cross section was observed. This cross section is similarly a result of performing chemical polishing of dipping the copper layer for 15 seconds in an aqueous solution of NH 3 :29%, H 2 O 2 :1%.
  • a drum-based one bath-type electroplating apparatus was used and a copper plated layer was formed with only one cell and with only one zone in order to reduce the number of zones. Specifically, there is only one copper layer.
  • this copper layer was etched to form a circuit, and a tin plated layer of approximately 0.3 ⁇ m was additionally formed on the copper circuit by dipping it into a tin plating bath of AT-501 manufactured by Nikko Mining & Metals at 50° C. for 3 minutes.
  • the copper layer was annealed at 125° C. ⁇ 10.5 hours, and the cross section was observed. This cross section is similarly a result of performing chemical polishing of dipping the copper layer for 15 seconds in an aqueous solution of NH 3 :29%, H 2 O 2 :1%.
  • a polyimide film was continuously introduced into conventional ten copper plating baths, and ten copper layers were formed on the surface of the polyimide film in a zigzag.
  • the observation of the Kirkendall voids are shown.
  • the average thickness of one layer was approximately 0.5 ⁇ m, and a copper layer of approximately 8 ⁇ m was formed as the ten copper plated layers.
  • FIG. 10 is a result of performing chemical polishing of dipping the copper layer for 15 seconds in an aqueous solution of NH 3 :29%, H 2 O 2 :1%.
  • the other conditions were the same as Example 1.
  • this copper layer was etched to form a circuit, and a tin plated layer of approximately 0.3 ⁇ m was additionally formed on the copper circuit by dipping it into a tin plating bath of AT-501 manufactured by Nikko Mining & Metals at 50° C. for 3 minutes.
  • the copper layer was annealed at 125° C. ⁇ 10.5 hours, and the cross section was observed. This cross section is similarly a result of performing chemical polishing of dipping the copper layer for 15 seconds in an aqueous solution of NH 3 :29%, H 2 O 2 :1%.
  • the number of abundant Kirkendall voids that arise in the ten copper layers is so high that peeling occurred between the copper layer and the tin plated layer.
  • the metal covered polyimide composite, method of producing the composite and apparatus for producing the composite of the present invention can effectively prevent peeling in a non-adhesive flexible laminate (especially a two-layer flexible laminate), particularly can effectively inhibit peeling from the interface of a copper layer and a tin plating, and yield a superior effect of being able to improve the adhesion strength.
  • the present invention is useful as a non-adhesive flexible laminate that is used as a mounting material of electronic components such as a flexible print substrate, TAB, COF.

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  • General Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Electroplating Methods And Accessories (AREA)
  • Laminated Bodies (AREA)
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  • Parts Printed On Printed Circuit Boards (AREA)
  • Manufacturing Of Printed Wiring (AREA)
US12/738,095 2007-10-18 2008-09-16 Metal Covered Polyimide Composite, Process for Producing the Composite, and Apparatus for Producing the Composite Abandoned US20100215982A1 (en)

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US8487191B2 (en) 2008-12-26 2013-07-16 Jx Nippon Mining & Metals Corporation Flexible laminate and flexible electronic circuit board formed by using the same
US8524378B2 (en) 2008-11-25 2013-09-03 Jx Nippon Mining & Metals Corporation Copper foil for printed circuit
WO2016205137A1 (en) * 2015-06-16 2016-12-22 3M Innovative Properties Company Plated polymeric article including tin/copper tie/seed layer
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JP5440410B2 (ja) * 2010-06-21 2014-03-12 住友金属鉱山株式会社 金属化樹脂フィルムの製造方法及び製造装置
KR101803165B1 (ko) * 2013-03-29 2017-11-29 제이엑스금속주식회사 캐리어 부착 동박, 프린트 배선판, 구리 피복 적층판, 전자 기기 및 프린트 배선판의 제조 방법
TWI573687B (zh) * 2013-12-31 2017-03-11 財團法人工業技術研究院 積層板及其製作方法
JP2019038136A (ja) * 2017-08-23 2019-03-14 住友金属鉱山株式会社 両面金属積層板及びその製造方法
CN110418512A (zh) * 2019-08-02 2019-11-05 合肥奕斯伟材料技术有限公司 一种提升COF Film耐折性的制作方法
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Cited By (10)

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US20100040873A1 (en) * 2006-11-29 2010-02-18 Nippon Mining & Metals Co., Ltd. Two-Layered Copper-Clad Laminate
US20100221563A1 (en) * 2007-10-18 2010-09-02 Nippon Mining And Metals Co., Ltd. Metal Covered Polyimide Composite, Process for Producing the Composite, and Process for Producing Electronic Circuit Board
US8568899B2 (en) * 2007-10-18 2013-10-29 Jx Nippon Mining & Metals Corporation Metal covered polyimide composite, process for producing the composite, and process for producing electronic circuit board
US20110233320A1 (en) * 2008-11-25 2011-09-29 Jx Nippon Mining & Metals Corporation Method of winding up copper foil or copper clad laminate
US8524378B2 (en) 2008-11-25 2013-09-03 Jx Nippon Mining & Metals Corporation Copper foil for printed circuit
US9992874B2 (en) 2008-12-24 2018-06-05 Jx Nippon Mining & Metals Corporation Metal foil with carrier
US8487191B2 (en) 2008-12-26 2013-07-16 Jx Nippon Mining & Metals Corporation Flexible laminate and flexible electronic circuit board formed by using the same
CN102209437A (zh) * 2010-10-19 2011-10-05 博罗县精汇电子科技有限公司 具有聚酰亚胺和铝基板复合结构的电路板及其制作方法
WO2016205137A1 (en) * 2015-06-16 2016-12-22 3M Innovative Properties Company Plated polymeric article including tin/copper tie/seed layer
US11066753B2 (en) 2015-06-16 2021-07-20 3M Innovative Properties Company Plated polymeric article including tin/copper tie/seed layer

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CN101827957A (zh) 2010-09-08
JPWO2009050970A1 (ja) 2011-03-03
US20120132531A1 (en) 2012-05-31
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TW200930561A (en) 2009-07-16

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