WO2020105289A1 - 表面処理銅箔、キャリア付銅箔、銅張積層板及びプリント配線板 - Google Patents

表面処理銅箔、キャリア付銅箔、銅張積層板及びプリント配線板

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Publication number
WO2020105289A1
WO2020105289A1 PCT/JP2019/038866 JP2019038866W WO2020105289A1 WO 2020105289 A1 WO2020105289 A1 WO 2020105289A1 JP 2019038866 W JP2019038866 W JP 2019038866W WO 2020105289 A1 WO2020105289 A1 WO 2020105289A1
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WO
WIPO (PCT)
Prior art keywords
copper foil
treated
resin
carrier
treated copper
Prior art date
Application number
PCT/JP2019/038866
Other languages
English (en)
French (fr)
Japanese (ja)
Inventor
翼 加藤
光由 松田
Original Assignee
三井金属鉱業株式会社
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by 三井金属鉱業株式会社 filed Critical 三井金属鉱業株式会社
Priority to JP2020558136A priority Critical patent/JP7453154B2/ja
Priority to KR1020217008111A priority patent/KR20210090608A/ko
Priority to CN201980073918.XA priority patent/CN112969824A/zh
Publication of WO2020105289A1 publication Critical patent/WO2020105289A1/ja

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Classifications

    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K3/00—Apparatus or processes for manufacturing printed circuits
    • H05K3/10—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
    • 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
    • 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
    • C25D5/16—Electroplating with layers of varying thickness
    • 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
    • C25D5/605—Surface topography of the layers, e.g. rough, dendritic or nodular 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
    • 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
    • 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
    • H05K1/09—Use of materials for the conductive, e.g. metallic pattern
    • 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
    • H05K3/025—Processes for manufacturing precursors of printed circuits, i.e. copper-clad substrates by transfer of thin metal foil formed on a temporary carrier, e.g. peel-apart copper
    • 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
    • H05K3/06—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 the conductive material being removed chemically or electrolytically, e.g. by photo-etch process
    • 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
    • H05K3/18—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 using precipitation techniques to apply the conductive material
    • 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

Definitions

  • the present invention relates to a surface-treated copper foil, a copper foil with a carrier, a copper-clad laminate, and a printed wiring board.
  • the SAP method is a method suitable for forming an extremely fine circuit, and one example thereof is a roughened copper foil with a carrier.
  • a carrier for example, as shown in FIGS. 1 and 2, an ultrathin copper foil 10 having a roughened surface is used, and a prepreg 12 and a primer layer 13 are used on an insulating resin substrate 11 having a lower layer circuit 11b on a base substrate 11a.
  • the carrier After pressing to bring them into close contact (step (a)), the carrier (not shown) is peeled off, and then via holes 14 are formed by laser drilling if necessary (step (b)).
  • the ultra-thin copper foil is removed by etching to expose the primer layer 13 provided with the roughened surface profile (step (c)).
  • electroless copper plating 15 is applied to this roughened surface (step (d))
  • it is masked with a predetermined pattern by exposure and development using a dry film 16 (step (e)), and electrolytic copper plating 17 is applied.
  • Step (f) After the dry film 16 is removed to form the wiring portion 17a (step (g)), the unnecessary electroless copper plating 15 between the adjacent wiring portions 17a, 17a is removed by etching (step (h)).
  • the wiring 18 formed in a predetermined pattern is obtained.
  • the roughened copper foil itself is removed by etching after laser perforation (step (c)). Then, since the uneven shape of the roughened surface of the roughened copper foil is transferred to the surface of the laminate from which the roughened copper foil has been removed, the insulating layer (for example, the primer layer 13 or the If not present, the adhesion between the prepreg 12) and the plating circuit (for example, the wiring 18) can be secured.
  • a modified semi-additive method which does not include the copper foil removing step corresponding to the step (c), is also widely used, but a copper foil is used in the etching step after removing the dry film (corresponding to the step (h)).
  • the MSAP method is somewhat inferior to the SAP method in the fine circuit formability because it is necessary to make the circuit space somewhat narrower in consideration of a larger etching amount. That is, the SAP method is more advantageous for the purpose of forming a finer circuit.
  • the interface between the circuit (for example, the wiring 18) and the insulating layer is etched, and as a result, the root of the circuit is eroded so as to be dug. A phenomenon called "plugging" may occur. When this insertion occurs, the adhesive force between the circuit and the insulating layer is reduced, causing the circuit to peel off.
  • a roughened copper foil in which the shape of roughened particles is controlled is known.
  • Patent Document 1 Japanese Patent No. 6293365
  • the average height of the substantially spherical protrusions is 2.60 ⁇ m or less
  • the ratio b ave / a ave of the average maximum diameter b ave of the substantially spherical protrusions is set to 1.2 or more, an excellent plating circuit is obtained when used in the SAP method. It is said that the laminate can be provided with a surface profile that is excellent not only in adhesiveness but also in etching properties for electroless copper plating.
  • the adoption of the SAP method which is advantageous for forming fine circuits, is expanding.
  • the allowable insertion width is relatively reduced as the circuit pattern width is narrowed.
  • an etching solution capable of selectively removing electroless copper instead of electrolytic copper can be used. ..
  • the SAP method is more advantageous than the MSAP method in terms of fine circuit formability.
  • the lowermost part of the circuit formed by the SAP method is made of electroless copper, when the above etching solution is used, insertion is more likely to occur.
  • the present inventors have recently provided a unique surface profile defined by the skewness Ssk measured according to ISO25178 on the surface of a resin base material, thereby performing an etching process of an electroless copper plating layer in the SAP method.
  • a surface-treated copper foil capable of imparting the above-mentioned specific surface profile to a resin substrate can be provided when used in the SAP method.
  • an object of the present invention is to provide a resin substrate with a surface profile capable of effectively suppressing the occurrence of insertion that may occur in a circuit in the step of etching an electroless copper plating layer when used in the SAP method.
  • a surface-treated copper foil To provide a surface-treated copper foil.
  • a surface-treated copper foil having a treated surface on at least one side Transfer the surface shape of the treated surface to the surface of the resin film by thermocompression bonding a resin film on the treated surface, and when the surface-treated copper foil is removed by etching, in the surface of the resin film left.
  • a surface-treated copper foil having a skewness Ssk of ⁇ 0.6 or less measured according to ISO25178 is provided.
  • the present invention comprising a carrier, a release layer provided on the carrier, and the surface-treated copper foil provided on the release layer with the treated surface outside. Copper foil with a carrier is provided.
  • a copper clad laminate provided with the surface-treated copper foil or the carrier-attached copper foil.
  • a printed wiring board obtained by using the surface-treated copper foil or the carrier-added copper foil.
  • a resin substrate in which at least one surface has a skewness Ssk measured according to ISO25178 of ⁇ 0.6 or less.
  • FIG. 9B is a diagram showing that the protrusion of the resin replica in the laminate of FIG. 9A is extracted and then the height of the protrusion is corrected. It is a figure which shows extracting the convex part of the resin replica in the laminated body of FIG. 9B, and performing height correction of a convex part. It is a figure for demonstrating the measuring method of the insertion amount.
  • the “skewness Ssk” is a parameter representing the symmetry of the height distribution measured according to ISO25178. When this value is 0, it means that the height distribution is vertically symmetrical. Further, as shown in FIG. 3A, when this value is smaller than 0, it indicates that the surface has many fine valleys. On the other hand, as shown in FIG. 3B, when the value is larger than 0, it means that the surface has many fine peaks.
  • the skewness Ssk can be calculated by measuring the surface profile of a predetermined measurement area (for example, a two-dimensional area of 57074.677 ⁇ m 2 ) on the treated surface with a commercially available laser microscope.
  • the "arithmetic mean curve Spc of mountain peak” is a parameter representing the arithmetic mean of the principal curvatures of the mountain peaks of the surface, measured according to ISO25178. If this value is small, it means that the point of contact with another object is rounded. On the other hand, if this value is large, it means that the point of contact with another object is sharp.
  • the arithmetic mean curve Spc at the peak is a parameter that can be measured by a laser microscope and that represents the roundness of the bump.
  • the arithmetic mean curve Spc at the peak can be calculated by measuring the surface profile of a predetermined measurement area (for example, a two-dimensional area of 57074.677 ⁇ m 2 ) on the treated surface with a commercially available laser microscope.
  • the "mountain peak density Spd” is a parameter representing the number of peaks per unit area, which is measured according to ISO25178. When this value is large, it suggests that there are many contact points with other objects.
  • the peak vertex density Spd can be calculated by measuring the surface profile of a predetermined measurement area (for example, a two-dimensional area of 57074.677 ⁇ m 2 ) on the treated surface with a commercially available laser microscope.
  • the “surface load curve” (hereinafter, simply referred to as “load curve”) is a curve representing the height at which the load area ratio is 0% to 100%, which is measured according to ISO25178.
  • the load area ratio is a parameter indicating the area of a region having a certain height c or more, as shown in FIG.
  • the load area ratio at the height c corresponds to Smr (c) in FIG.
  • the secant of the load curve obtained by subtracting the difference of the load area rates from the load area rate of 0% along the load curve to 40% is moved from the load area rate of 0% to the secant line.
  • the position where the slope of the load becomes the gentlest is called the central part of the load curve.
  • a straight line that minimizes the sum of squared deviations in the vertical axis with respect to the central portion is called an equivalent straight line.
  • the portion included in the range of the load area ratio of the equivalent straight line from 0% to 100% is called the core portion.
  • a portion higher than the core portion is called a protruding peak portion, and a portion lower than the core portion is called a protruding valley portion.
  • the core portion represents the height of the area in contact with another object after the initial wear is finished.
  • the “pole height Sxp” is a parameter representing the difference between the heights of the load area ratio p% and the load area ratio q%, which is measured according to ISO25178, as shown in FIG. is there.
  • Sxp represents the difference between the average surface of the surface and the height of the surface after removing particularly high peaks in the surface.
  • Sxp represents the difference in height between the load area ratio of 2.5% and the load area ratio of 50%.
  • the pole height Sxp can be calculated by measuring the surface profile of a predetermined measurement area (for example, a two-dimensional area of 57074.677 ⁇ m 2 ) on the treated surface with a commercially available laser microscope.
  • the "load area ratio Smr1 for separating the protruding peak portion and the core portion” means the intersection of the height of the upper portion of the core portion and the load curve measured according to ISO25178, as shown in FIG. Is a parameter indicating the load area ratio (that is, the load area ratio separating the core portion and the protruding mountain portion). The larger this value is, the larger the proportion occupied by the protruding mountain portion is.
  • the “load area ratio Smr2 for separating the protruding valley portion and the core portion” is, as shown in FIG. 5, the height of the lower portion of the core portion and the load curve measured according to ISO25178.
  • the “substantial volume Vmc of the core portion” is a parameter representing the volume of the core portion, which is measured according to ISO25178. As shown in FIG. 7, Vmc is the difference between the actual volume at the load area ratio Smr2 that separates the protruding valley portion and the core portion from the actual volume at the load area ratio Smr1 that separates the protruding mountain portion and the core portion. Represents.
  • the actual volume Vmc of the core portion can be calculated by measuring the surface profile of a predetermined measurement area (for example, a two-dimensional area of 57074.677 ⁇ m 2 ) on the treated surface with a commercially available laser microscope.
  • the load area ratio Smr1 for separating the protruding peak portion and the core portion is designated as 10%
  • the load area ratio Smr2 for separating the protruding valley portion and the core portion is designated as 80%, respectively
  • the actual volume Vmc of the core portion is specified. Shall be calculated.
  • the “electrode surface” of the electrolytic copper foil refers to the surface that is in contact with the cathode when the electrolytic copper foil is manufactured.
  • the “deposited surface” of the electrolytic copper foil refers to the surface on which electrolytic copper is deposited during production of the electrolytic copper foil, that is, the surface not in contact with the cathode.
  • the copper foil according to the present invention is a surface-treated copper foil.
  • This surface-treated copper foil is a resin film that remains when the surface shape of the treated surface is transferred to the surface of the resin film by thermocompression bonding the resin film to the treated surface and the surface-treated copper foil is removed by etching (hereinafter , And also referred to as a resin replica) (hereinafter, also referred to as a transfer surface) has a skewness Ssk measured according to ISO 25178 of ⁇ 0.6 or less.
  • the adoption of the SAP method which is advantageous for forming fine circuits, is expanding with the demand for further miniaturization of circuits.
  • the allowable insertion width is relatively reduced as the circuit pattern width is narrowed. That is, the insertion width, which has been allowed in the conventional pattern width (for example, 30 ⁇ m), may deviate from the standard due to an increased risk of circuit collapse in a finer circuit pattern width (for example, 10 ⁇ m).
  • the SAP method is advantageous in terms of circuit miniaturization compared to other construction methods such as the MSAP method, it may be disadvantageous in terms of suppressing insertion.
  • a laminate in which a rust preventive layer 114 derived from a copper foil with a carrier and an electrolytic copper layer 116 are sequentially laminated on a resin substrate 112. 110 is prepared (step (i)), and electroless copper plating 118 is formed while the electrolytic copper layer 116 remains.
  • a dry film is used for masking in a predetermined pattern, and then electrolytic copper plating is performed to form the wiring portion 120 (step (ii)).
  • the electrolytic copper layer 116 remains on the resin base material 112
  • the electrolytic copper layer 116 and the electroless copper layer are removed in the step of etching and removing the unnecessary portion between the adjacent wiring portions 120 and 120.
  • the two layers of plating 118 must be etched away. Therefore, as shown in step (iii) of FIG. 8A, the obtained wiring 122 is likely to have a circuit thinning.
  • the electrolytic copper layer 116 is not completely removed as described above, the rust preventive layer 114 exists between the resin base material 112 and the wiring 122, and the rust preventive layer 114 is inserted.
  • step (i ) preparation of the laminated body 110 in which the rust preventive layer 114 and the electrolytic copper layer 116 are sequentially formed on the resin substrate 112 (step (i )), Complete removal of the electrolytic copper layer 116 (step (ii)), formation of the electroless copper plating 118, masking with a dry film, and formation of the wiring portion 120 by electrolytic copper plating (step (iii)).
  • the electrolytic copper layer 116 does not remain on the resin base material 112. Therefore, in the etching process of the unnecessary portion between the adjacent wiring portions 120, 120, only the electroless copper plating 118 is removed by etching.
  • the SAP method since it is possible to use an etching solution that can selectively remove electroless copper instead of electrolytic copper, it is even more effective to reduce the thickness of the wiring 122 that is mostly composed of electrolytic copper. Can be suppressed to. Therefore, it can be said that the SAP method is more advantageous than other construction methods such as the MSAP method for miniaturization of the circuit.
  • the etching capable of selectively removing the electroless copper is performed.
  • the insertion 124 is likely to occur at the interface between the wiring 122 and the resin base material 112.
  • the electrolytic copper layer 116 is completely removed by etching in the SAP method.
  • the rust preventive metal is also etched during the etching (see step (ii) in FIG. 8B). 8A and 8B, the thickness of the anticorrosion layer 114 is shown large for emphasis, and does not necessarily reflect the actual thickness ratio of the laminate. As described above, in the SAP method, it is not easy to suppress the insertion that may occur in the circuit.
  • the surface-treated copper foil of the present invention for the SAP method, it is possible to impart a unique surface profile with a skewness Ssk measured according to ISO25178 of ⁇ 0.6 or less on the surface of the resin substrate. it can. By doing so, it is possible to effectively suppress the occurrence of insertion that may occur in the circuit in the step of etching the electroless copper plating layer.
  • the mechanism by which the resin base material surface has the above-mentioned surface profile to suppress the insertion that occurs in the circuit is not always clear, but one of the factors is as follows.
  • the convex portion of the surface of the resin base material on which the circuit is formed functions as a protective wall for preventing the intrusion of the etching solution in the etching step of the electroless copper plating in the SAP method. Therefore, it can be said that the thicker this protective wall, the less likely it is that insertion will occur.
  • the resin replica 20 having the small skewness Ssk is the resin replica 20 having the large skewness Ssk (see FIG. 9B).
  • the wall thickness of the convex portion 20a is thicker than that of the convex portion 20a (see the circled portions in the drawing). Therefore, it is considered that by making the skewness Ssk of the resin replica as small as ⁇ 0.6 or less, it is possible to thicken the protective wall, and thus to effectively suppress the insertion in the circuit 22. ..
  • the surface-treated copper foil of the present invention is preferably used for producing a printed wiring board by the SAP method.
  • the surface-treated copper foil of the present invention is preferably used for transferring the uneven shape to the insulating resin layer for the printed wiring board.
  • the surface-treated copper foil of the present invention has a treated surface on at least one side.
  • the treated surface is a surface that has been subjected to some kind of surface treatment, and is typically a roughened surface.
  • the treated surface typically comprises a plurality of bumps (eg, roughened particles).
  • the surface-treated copper foil may have a treated surface (for example, a roughened surface) on both sides, or may have a treated surface on only one side.
  • the surface on the laser irradiation side (the surface on the opposite side to the surface to be brought into close contact with the insulating resin) is also surface-treated when used in the SAP method, so that the laser absorptivity is enhanced. As a result, the laser piercing property can also be improved.
  • the surface-treated copper foil of the present invention is a resin film left when the surface shape of the treated surface is transferred to the surface of the resin film by thermocompression bonding the resin film to the treated surface and the surface-treated copper foil is removed by etching.
  • the bumps on the treated surface of the surface-treated copper foil can be controlled to an appropriate shape that is not too elongated, while further suppressing the occurrence of insertion in the etching step of the SAP method, and thereby the surface can be controlled. It is possible to effectively suppress the occurrence of powder falling due to breakage or falling of the bumps in the treated copper foil.
  • the resin film is preferably a thermosetting resin film, and may be in the form of prepreg. Examples of the thermosetting resin include epoxy resin, cyanate resin, bismaleimide triazine resin (BT resin), polyphenylene ether resin, phenol resin, polyimide resin and the like.
  • thermocompression bonding is not particularly limited as long as the uneven shape of the treated surface of the surface-treated copper foil can be transferred to the resin film.
  • the surface of the resin film left after the etching is the arithmetic mean songs Spc summit point not more than 5000 mm -1 or higher 13000Mm -1 preferably , more preferably 7000 mm -1 or more 13000Mm -1 or less, more preferably 9000 mm -1 or more 13000Mm -1 or less, particularly preferably not more than 10000 mm -1 or more 13000mm -1.
  • the cobb on the treated surface of the surface-treated copper foil is controlled to an appropriate shape that is not too long and slender, and the occurrence of powder falling due to breakage or falling off of the cobb in the surface-treated copper foil is effectively performed. While suppressing, it is possible to further suppress the occurrence of insertion in the etching process of the SAP method.
  • One of the factors that can suppress the occurrence of insertion is as follows. That is, based on the definition of the arithmetic mean curve Spc of the mountain peak described above, as shown in FIGS. 9A and 9B, the resin replica 20 (see FIG. 9A) having a small arithmetic mean curve Spc of the mountain peak is the arithmetic of the mountain peak.
  • the peaks of the convex portions 20a are flat. As a result, it is considered that the wall thickness of the convex portion 20a that functions as the insertion protection wall becomes thick.
  • the surface of the resin film left after the etching (that is, the transfer surface of the resin replica) has a peak apex density Spd of 1.13 ⁇ 10 6 mm ⁇ 2 or more and 1.50 ⁇ 10 5. It is preferably 6 mm ⁇ 2 or less, more preferably 1.13 ⁇ 10 6 mm ⁇ 2 or more and 1.40 ⁇ 10 6 mm ⁇ 2 or less, still more preferably 1.14 ⁇ 10 6 mm ⁇ 2 or more 1. It is 30 ⁇ 10 6 mm ⁇ 2 or less, particularly preferably 1.15 ⁇ 10 6 mm ⁇ 2 or more and 1.20 ⁇ 10 6 mm ⁇ 2 or less.
  • the surface of the resin film left after the etching (that is, the transfer surface of the resin replica) has a substantial volume Vmc (mL / m 2 ) of the core portion with respect to the pole height Sxp ( ⁇ m).
  • the ratio Vmc / Sxp is preferably 0.39 or more and 0.44 or less, more preferably 0.39 or more and 0.43 or less, still more preferably 0.39 or more and 0.42 or less, and particularly preferably 0. It is 39 or more and 0.41 or less, and most preferably 0.39 or more and 0.40 or less.
  • the cobb on the treated surface of the surface-treated copper foil is controlled to an appropriate shape that is not too long and slender, and the occurrence of powder falling due to breakage or falling off of the cobb in the surface-treated copper foil is effectively performed. While suppressing, the occurrence of insertion in the etching process of the SAP method can be further suppressed. In addition, it is possible to increase the adhesion between the substrate and the circuit. That is, as described above, the convex portion of the resin replica functions as a protective wall that blocks the intrusion of the etching solution. Based on the definition of the actual volume Vmc of the core portion, the larger the actual volume Vmc of the core portion is, the larger the resin replica becomes.
  • the convex part of is also enlarged and the insertion is further suppressed.
  • the physical volume Vmc of the core portion is equal to the height of the convex portion 20a of the resin replica 20. Since Vmc / Sxp divided by the pole height Sxp, which is a parameter related to the height of the convex portion 20a, is compared, the convex portion 20a is obtained as a converted value in which the heights of the convex portions 20a are uniformly arranged. The size of can be evaluated.
  • Vmc / Sxp for example, 0.39 or more
  • the area of the convex portion 20a of the resin replica 20 that bites into the circuit 22 also increases (that is, the amount of resin surrounded and held by the circuit 22 increases. Therefore, the improvement of the anchor effect also increases the adhesion between the substrate and the circuit.
  • the surface-treated copper foil according to the present invention is not limited to the method described below, the surface described above on the resin film surface. It may be manufactured by any method as long as it can be profiled.
  • the thickness of the copper foil is not particularly limited, but is preferably 0.1 ⁇ m or more and 18 ⁇ m or less, more preferably 0.5 ⁇ m or more and 10 ⁇ m or less, further preferably 0.5 ⁇ m or more and 7 ⁇ m or less, particularly preferably 0.5 ⁇ m or more and 5 ⁇ m or less, Most preferably, it is 0.5 ⁇ m or more and 3 ⁇ m or less.
  • the copper foil is prepared in the form of a carrier-attached copper foil
  • the copper foil is a wet film forming method such as an electroless copper plating method and an electrolytic copper plating method, a dry film forming method such as sputtering and chemical vapor deposition, or It may be formed by a combination thereof.
  • the copper concentration is 5 g / L or more and 20 g / L or less
  • the sulfuric acid concentration is 30 g / L or more and 200 g / L or less
  • the chlorine concentration is 20 mg / L or more and 100 mg / L or less
  • the 9-phenylacridine (9PA) concentration is Using a copper sulfate solution containing 20 mg / L or more and 80 mg / L or less, at a plating temperature of 20 ° C. or more and 40 ° C. or less, a current density of 5 A / dm 2 or more and 25 A / dm 2 or less, and a time of 2 seconds or more and 10 seconds or less. It is preferable to perform electrodeposition.
  • This first stage plating process may be performed twice in total using two tanks, but it is preferable to complete the plating process once in total.
  • a copper sulfate solution containing a copper concentration of 65 g / L or more and 80 g / L or less and a sulfuric acid concentration of 200 g / L or more and 280 g / L or less is used, and the liquid temperature is 45 ° C. or more and 55 ° C. or less and the current density is 1 A. It is preferable to perform electrodeposition under the plating conditions of / dm 2 or more and 10 A / dm 2 or less and time of 2 seconds or more and 25 seconds or less.
  • the copper concentration is 10 g / L or more and 20 g / L or less
  • the sulfuric acid concentration is 30 g / L or more and 130 g / L or less
  • the chlorine concentration is 20 mg / L or more and 100 mg / L or less
  • the 9PA concentration is 100 mg / L or more and 200 mg / L.
  • the first-stage plating process be performed using an additive such as 9PA, etc., and the total amount of electricity Q 1 in the first-stage plating process and the total amount of electricity Q 2 in the second-stage plating process It is preferable to set the amount (Q 1 + Q 2 ) to 100 C / dm 2 or less.
  • the distance between the positive electrode and the negative electrode in the first plating step is preferably 45 mm or more and 90 mm or less, and more preferably 50 mm or more and 80 mm or less.
  • the anticorrosion treatment preferably includes a plating treatment using zinc.
  • the plating treatment using zinc may be either a zinc plating treatment or a zinc alloy plating treatment, and the zinc alloy plating treatment is particularly preferably a zinc-nickel alloy treatment.
  • the zinc-nickel alloy treatment may be a plating treatment containing at least Ni and Zn, and may further contain other elements such as Sn, Cr and Co.
  • the Ni / Zn adhesion ratio in the zinc-nickel alloy plating is preferably 1.2 or more and 10 or less, more preferably 2 or more and 7 or less, still more preferably 2.7 or more and 4 or less in terms of mass ratio.
  • the anticorrosion treatment preferably further includes a chromate treatment, and this chromate treatment is more preferably performed on the surface of the zinc-containing plating after the zinc plating treatment.
  • a particularly preferred anticorrosion treatment is a combination of a zinc-nickel alloy plating treatment and a subsequent chromate treatment.
  • the copper foil may be treated with a silane coupling agent to form a silane coupling agent layer.
  • a silane coupling agent layer can be formed by appropriately diluting and applying the silane coupling agent and then drying.
  • silane coupling agents include epoxy-functional silane coupling agents such as 4-glycidylbutyltrimethoxysilane and 3-glycidoxypropyltrimethoxysilane, or 3-aminopropyltriethoxysilane, N-2 (amino).
  • Silane coupling agent mercapto-functional silane coupling agent such as 3-mercaptopropyltrimethoxysilane, or olefin-functional silane coupling agent such as vinyltrimethoxysilane, vinylphenyltrimethoxysilane, or 3-methacryloxypropyl
  • acrylic functional silane coupling agents such as trimethoxysilane
  • imidazole functional silane coupling agents such as imidazole silane
  • triazine functional silane coupling agents such as triazine silane.
  • the surface-treated copper foil of the present invention can be provided in the form of a copper foil with a carrier.
  • the carrier-attached copper foil comprises a carrier, a release layer provided on the carrier, and a treated surface (typically a roughened surface) provided on the release layer of the present invention.
  • a surface-treated copper foil typically a roughened surface
  • the carrier-added copper foil may have a known layer configuration except that the surface-treated copper foil of the present invention is used.
  • the carrier is a layer (typically a foil) for supporting the surface-treated copper foil and improving its handling property.
  • the carrier include an aluminum foil, a copper foil, a resin film whose surface is metal-coated with copper or the like, a glass plate, and the like, and a copper foil is preferable.
  • the copper foil may be either a rolled copper foil or an electrolytic copper foil.
  • the thickness of the carrier is typically 200 ⁇ m or less, preferably 12 ⁇ m or more and 35 ⁇ m or less.
  • the release layer side surface of the carrier preferably has a ten-point surface roughness Rz of 0.5 ⁇ m or more and 1.5 ⁇ m or less, more preferably 0.6 ⁇ m or more and 1.0 ⁇ m or less.
  • Rz can be determined according to JIS B 0601-1994.
  • the peeling layer is a layer having a function of weakening the peeling strength of the carrier, ensuring stability of the strength, and suppressing interdiffusion that may occur between the carrier and the copper foil during press molding at high temperature. ..
  • the release layer is generally formed on one surface of the carrier, but may be formed on both surfaces.
  • the release layer may be either an organic release layer or an inorganic release layer.
  • organic components used in the organic release layer include nitrogen-containing organic compounds, sulfur-containing organic compounds, and carboxylic acids.
  • the nitrogen-containing organic compound include a triazole compound and an imidazole compound. Among them, the triazole compound is preferable because the peelability is easily stabilized.
  • Examples of the triazole compound include 1,2,3-benzotriazole, carboxybenzotriazole, N ′, N′-bis (benzotriazolylmethyl) urea, 1H-1,2,4-triazole and 3-amino- 1H-1,2,4-triazole and the like can be mentioned.
  • Examples of the sulfur-containing organic compound include mercaptobenzothiazole, thiocyanuric acid, 2-benzimidazole thiol and the like.
  • Examples of the carboxylic acid include monocarboxylic acid and dicarboxylic acid.
  • examples of inorganic components used in the inorganic release layer include Ni, Mo, Co, Cr, Fe, Ti, W, P, Zn, and chromate-treated films.
  • the release layer may be formed by bringing a release layer component-containing solution into contact with at least one surface of the carrier and fixing the release layer component on the surface of the carrier.
  • the contact of the carrier with the release layer component-containing solution may be performed by immersing the carrier in the release layer component-containing solution, spraying the release layer component-containing solution, flowing down the release layer component-containing solution, and the like.
  • the release layer component may be fixed to the carrier surface by adsorption or drying of the release layer component-containing solution, electrodeposition of the release layer component in the release layer component-containing solution, or the like.
  • the thickness of the peeling layer is typically 1 nm or more and 1 ⁇ m or less, preferably 5 nm or more and 500 nm or less.
  • the above-mentioned surface-treated copper foil of the present invention is used as the surface-treated copper foil.
  • the roughening treatment of the present invention is a roughening treatment using copper particles.
  • a copper layer is formed as a copper foil on the surface of the release layer, and then at least roughening may be performed. ..
  • the details of roughening are as described above.
  • the copper foil is preferably formed in the form of an ultrathin copper foil in order to take advantage of the advantages of the copper foil with a carrier.
  • the thickness of the ultrathin copper foil is preferably 0.1 ⁇ m or more and 7 ⁇ m or less, more preferably 0.5 ⁇ m or more and 5 ⁇ m or less, and further preferably 0.5 ⁇ m or more and 3 ⁇ m or less.
  • Another functional layer may be provided between the peeling layer and the carrier and / or the copper foil.
  • Examples of such other functional layers include auxiliary metal layers.
  • the auxiliary metal layer preferably comprises nickel and / or cobalt.
  • the thickness of the auxiliary metal layer is preferably 0.001 ⁇ m or more and 3 ⁇ m or less.
  • Copper- clad laminate The surface-treated copper foil or copper foil with a carrier of the present invention is preferably used for producing a copper-clad laminate for a printed wiring board. That is, according to a preferred aspect of the present invention, there is provided a copper clad laminate provided with the surface-treated copper foil or the carrier-attached copper foil. By using the surface-treated copper foil or the copper foil with a carrier of the present invention, it is possible to provide a copper-clad laminate which is particularly suitable for the SAP method.
  • This copper clad laminate comprises the surface-treated copper foil of the present invention and a resin layer provided in close contact with the roughened surface of the surface-treated copper foil, or a copper foil with a carrier of the present invention And a resin layer provided in close contact with the roughening-treated surface of the surface-treated copper foil in the carrier-added copper foil.
  • the surface-treated copper foil or the carrier-added copper foil may be provided on one side or both sides of the resin layer.
  • the resin layer comprises a resin, preferably an insulating resin.
  • the resin layer is preferably a prepreg and / or a resin sheet.
  • the prepreg is a general term for composite materials obtained by impregnating a base material such as a synthetic resin plate, a glass plate, a glass woven cloth, a glass non-woven cloth, and paper with a synthetic resin.
  • a base material such as a synthetic resin plate, a glass plate, a glass woven cloth, a glass non-woven cloth, and paper
  • a synthetic resin such as a synthetic resin plate, a glass plate, a glass woven cloth, a glass non-woven cloth, and paper with a synthetic resin.
  • the insulating resin include epoxy resin, cyanate resin, bismaleimide triazine resin (BT resin), polyphenylene ether resin, and phenol resin.
  • examples of the insulating resin that constitutes the resin sheet include insulating resins such as epoxy resin, polyimide resin, and polyester resin.
  • the resin layer may contain filler particles made of various inorganic particles such as silica and alumina from the viewpoint of improving the insulating property.
  • the thickness of the resin layer is not particularly limited, but is preferably 1 ⁇ m or more and 1000 ⁇ m or less, more preferably 2 ⁇ m or more and 400 ⁇ m or less, and further preferably 3 ⁇ m or more and 200 ⁇ m or less.
  • the resin layer may be composed of a plurality of layers.
  • a resin layer such as a prepreg and / or a resin sheet may be provided on the surface-treated copper foil or the carrier-added copper foil via a primer resin layer which is applied to the roughened surface of the surface-treated copper foil in advance.
  • the surface-treated copper foil or copper foil with a carrier of the present invention is preferably used for producing a printed wiring board, and particularly preferably used for producing a printed wiring board by a semi-additive method (SAP). That is, according to a preferred embodiment of the present invention, a printed wiring board is manufactured by using the above-mentioned surface-treated copper foil or the above-mentioned carrier-attached copper foil, a method for manufacturing a printed wiring board, or the above-mentioned surface treatment. There is provided a printed wiring board obtained by using a copper foil or the above-mentioned copper foil with a carrier.
  • SAP semi-additive method
  • the printed wiring board according to this aspect includes a layer structure in which a resin layer and a copper layer are laminated.
  • the surface-treated copper foil of the present invention is removed in the step (c) of FIG. 1, the printed wiring board produced by the SAP method no longer contains the surface-treated copper foil of the present invention. Only the surface profile transferred from the roughened surface of the treated copper foil remains.
  • the resin layer is as described above for the copper clad laminate.
  • the printed wiring board may have a known layer structure.
  • Specific examples of the printed wiring board a single-sided or double-sided printed wiring board formed into a circuit on a laminate obtained by adhering the surface-treated copper foil or the copper foil with a carrier of the present invention to one side or both sides of the prepreg and curing it, and these.
  • Examples include a multilayer printed wiring board in which the above is multilayered.
  • other specific examples include a flexible printed wiring board, a COF, a TAB tape, etc. in which a surface-treated copper foil or a copper foil with a carrier of the present invention is formed on a resin film to form a circuit.
  • a resin-coated copper foil obtained by applying the resin layer to the surface-treated copper foil or the carrier-coated copper foil of the present invention is formed, and the resin layer is used as an insulating adhesive layer to form the above-mentioned print.
  • the surface-treated copper foil is used as the whole or a part of the wiring layer to remove the build-up wiring board on which the circuit is formed by the modified semi-additive (MSAP) method, the subtractive method, etc., and the surface-treated copper foil.
  • MSAP modified semi-additive
  • a build-up wiring board in which a circuit is formed by a semi-additive (SAP) method, a direct build-up-on-wafer in which a resin-coated copper foil is laminated and a circuit is alternately formed on a semiconductor integrated circuit are listed.
  • SAP semi-additive
  • an antenna element formed by laminating the above resin-coated copper foil on a base material to form a circuit an electronic material for a panel display or a window formed by laminating on a glass or resin film through an adhesive layer to form a pattern
  • Examples also include electronic materials for glass, electromagnetic wave shield films obtained by coating the surface-treated copper foil of the present invention with a conductive adhesive, and the like.
  • the surface-treated copper foil or the copper foil with a carrier of the present invention is suitable for the SAP method.
  • the configurations shown in FIGS. 1 and 2 can be adopted.
  • a resin base material in which at least one surface has a skewness Ssk of ⁇ 0.6 or less measured according to ISO25178.
  • This resin base material corresponds to a resin replica on which the surface shape of the surface-treated copper foil of the present invention is transferred. Therefore, a preferred embodiment of the resin replica in which the surface shape of the above-mentioned surface-treated copper foil is transferred (skewness Ssk, arithmetic mean curve Spc of peaks, density of peaks Spd of peaks, and substantial volume Vmc of core with respect to pole height Sxp).
  • the respective parameters of the ratio Vmc / Sxp) of (1) apply to the resin base material of this embodiment as they are.
  • the resin substrate comprises a resin, preferably an insulating resin.
  • the resin base material is preferably a prepreg and / or a resin sheet.
  • the prepreg is a general term for composite materials obtained by impregnating a base material such as a synthetic resin plate, a glass plate, a glass woven cloth, a glass non-woven cloth, and paper with a synthetic resin.
  • a base material such as a synthetic resin plate, a glass plate, a glass woven cloth, a glass non-woven cloth, and paper
  • the insulating resin include epoxy resin, cyanate resin, bismaleimide triazine resin (BT resin), polyphenylene ether resin, and phenol resin.
  • examples of the insulating resin that constitutes the resin base material include insulating resins such as epoxy resin, polyimide resin, and polyester resin.
  • the resin base material may contain filler particles made of various inorganic particles such as silica and alumina from the viewpoint of improving the insulating property.
  • the thickness of the resin substrate is not particularly limited, but is preferably 1 ⁇ m or more and 1000 ⁇ m or less, more preferably 2 ⁇ m or more and 400 ⁇ m or less, and further preferably 3 ⁇ m or more and 200 ⁇ m or less.
  • the resin substrate may be composed of a plurality of layers.
  • the resin base material of the present invention can be preferably used as a starting material or an intermediate product in the production of a printed wiring board by the SAP method.
  • Examples 1-6 The copper foil with a carrier and the resin replica were produced and evaluated as follows.
  • the electrode surface side of the pickled carrier was immersed in a CBTA aqueous solution having a CBTA (carboxybenzotriazole) concentration of 1 g / L, a sulfuric acid concentration of 150 g / L and a copper concentration of 10 g / L at a liquid temperature of 30 ° C. Was immersed for 30 seconds, and the CBTA component was adsorbed on the electrode surface of the carrier.
  • the CBTA layer was formed as an organic release layer on the surface of the electrode surface of the carrier.
  • the carrier having the organic release layer formed thereon is dipped in a solution of nickel sulfate having a nickel concentration of 20 g / L to obtain a liquid temperature of 45 ° C., a pH of 3, and a current density of 5 A / dm. Under the condition of 2, the amount of nickel corresponding to the thickness of 0.001 ⁇ m was deposited on the organic release layer. Thus, a nickel layer was formed as an auxiliary metal layer on the organic release layer.
  • the carrier on which the auxiliary metal layer is formed is immersed in a copper sulfate solution having a copper concentration of 60 g / L and a sulfuric acid concentration of 200 g / L to obtain a solution temperature of 50 ° C. and a current density of 5 A / dm 2 or more. Electrolysis was performed at 30 A / dm 2 or less to form an ultrathin copper foil having a thickness of 1.2 ⁇ m on the auxiliary metal layer.
  • Roughening treatment A roughening treatment was performed on the deposition surface of the ultrathin copper foil described above. In this roughening treatment, the plating in the first step was performed twice. In the plating process at each stage, a copper sulfate solution having a copper concentration, a sulfuric acid concentration, a chlorine concentration and a 9-phenylacridine (9PA) concentration shown in Table 1 was used, and at the liquid temperature shown in Table 1, the current density shown in Table 2 was used. And electrodeposition were carried out at different times. The distance between the positive electrode and the negative electrode in the plating treatment in the first step was 50 mm or more and 80 mm or less. Thus, six types of roughened copper foils of Examples 1 to 6 were produced.
  • Silane coupling agent treatment A silane coupling agent is prepared by adsorbing an aqueous solution containing 3-aminopropyltrimethoxysilane 3 g / L on the surface of the copper foil with carrier on the copper foil side and evaporating the water by an electric heater. Processed. At this time, the silane coupling agent treatment was not performed on the carrier side.
  • a copper clad laminate was prepared using a copper foil with a carrier.
  • an ultra-thin copper foil with a carrier was laminated on the surface of the inner layer substrate via a BT resin prepreg (Mitsubishi Gas Chemical Co., Inc., GHPL-830NS, thickness 0.1 mm) as a resin film, and pressure 4 After thermocompression bonding at 0.0 MPa and a temperature of 220 ° C. for 90 minutes, the carrier was peeled off to prepare a copper clad laminate.
  • BT resin prepreg Mitsubishi Gas Chemical Co., Inc., GHPL-830NS, thickness 0.1 mm
  • a circuit having a circuit width of 22 ⁇ m, a height of 22 ⁇ m, and a length of 150 ⁇ m is obtained by pasting a dry film on the surface of the SAP evaluation laminate, exposing it, removing the dry film, and electrolytic plating. The lower part is in a state of being electrically connected by an electroless copper plating layer).
  • the obtained circuit was treated with an etching solution (SAC-700W3C, manufactured by Ebara-Udylite Co., Ltd.) to dissolve and remove the electroless copper-plated layer remaining between the circuits to insulate each circuit.
  • the amount of etching at this time was performed under the condition of so-called over-etching, in which the etching rate of the copper foil was measured in advance and etching was performed by 4 ⁇ m more than so-called just etching.
  • the circuit was washed with water and dried.
  • the cross section of the circuit was observed using an optical microscope to determine the insertion amount. Specifically, as shown in FIG. 11, the upper width x ( ⁇ m) and the lower width y ( ⁇ m) of the circuit 22 formed on the resin replica 20 are measured, and the difference (xy) is calculated.
  • the measurement was carried out in two visual fields for each example, and the average value was used as the insertion amount of each example. The results are as shown in Table 3.
  • Example 5 Although the value of Vmc / Sxp is large, the peel strength does not increase so much. The reason for this is considered to be that "powder drop" is one factor. That is, when powder drop occurs, the anchor effect is no longer obtained and the peel strength tends to decrease, but powder drop occurs when Vmc / Sxp is too large. In Example 5, a slight powder drop occurred, so it is considered that the peel strength remains slightly low.

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PCT/JP2019/038866 2018-11-19 2019-10-02 表面処理銅箔、キャリア付銅箔、銅張積層板及びプリント配線板 WO2020105289A1 (ja)

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JP7174869B1 (ja) 2021-07-19 2022-11-17 長春石油化學股▲分▼有限公司 表面処理銅箔および銅クリッドラミネート
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JP2023014971A (ja) * 2021-07-19 2023-01-31 長春石油化學股▲分▼有限公司 表面処理銅箔および銅クリッドラミネート
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