WO2021157362A1 - Feuille de cuivre traitée par rugosification, feuille de cuivre avec support, carte stratifiée cuivrée, et carte de circuit imprimé - Google Patents

Feuille de cuivre traitée par rugosification, feuille de cuivre avec support, carte stratifiée cuivrée, et carte de circuit imprimé Download PDF

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Publication number
WO2021157362A1
WO2021157362A1 PCT/JP2021/001902 JP2021001902W WO2021157362A1 WO 2021157362 A1 WO2021157362 A1 WO 2021157362A1 JP 2021001902 W JP2021001902 W JP 2021001902W WO 2021157362 A1 WO2021157362 A1 WO 2021157362A1
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Prior art keywords
copper foil
roughened
less
carrier
filter
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PCT/JP2021/001902
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English (en)
Japanese (ja)
Inventor
眞 細川
哲聡 ▲高▼梨
美智 溝口
Original Assignee
三井金属鉱業株式会社
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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 CN202180012213.4A priority Critical patent/CN115038819A/zh
Priority to KR1020227022468A priority patent/KR20220106200A/ko
Priority to JP2021575705A priority patent/JP7259093B2/ja
Publication of WO2021157362A1 publication Critical patent/WO2021157362A1/fr

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    • 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
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/20—Layered products comprising a layer of metal comprising aluminium or copper
    • 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
    • C25D5/16—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
    • C25D5/48—After-treatment of electroplated surfaces
    • 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
    • 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
    • C23C2222/00—Aspects relating to chemical surface treatment of metallic material by reaction of the surface with a reactive medium
    • C23C2222/20—Use of solutions containing silanes

Definitions

  • the present invention relates to a roughened copper foil, a copper foil with a carrier, a copper-clad laminate, and a printed wiring board.
  • the MSAP method is a method suitable for forming an extremely fine circuit, and is performed using a copper foil with a carrier in order to take advantage of its characteristics.
  • the ultrathin copper foil 10 is pressed and adhered to the insulating resin substrate 11 provided with the lower layer circuit 11b on the base material 11a by using the prepreg 12 and the primer layer 13.
  • the carrier (not shown) is peeled off, and then a via hole 14 is formed by laser perforation if necessary (step (b)).
  • step (c) After the chemical copper plating 15 is applied (step (c)), masking is performed in a predetermined pattern by exposure and development using the dry film 16 (step (d)), and the electrolytic copper plating 17 is applied (step (e). )).
  • step (f) After removing the dry film 16 to form the wiring portion 17a (step (f)), unnecessary ultrathin copper foil and the like between the wiring portions 17a and 17a adjacent to each other are removed by etching over their entire thickness (step (f)).
  • Step (g) a wiring 18 formed in a predetermined pattern is obtained.
  • Patent Document 1 Patent No. 6462961
  • a roughening treatment layer, a rust prevention treatment layer and a silane coupling layer are provided on at least one surface of the copper foil.
  • Surface-treated copper foils laminated in this order are disclosed.
  • Patent Document 1 describes the development area ratio Sdr of the interface measured from the surface of the silane coupling layer of the surface-treated copper foil for the purpose of producing a printed wiring board having low transmission loss and excellent reflow heat resistance. It is also disclosed that the root mean square surface gradient Sdq is 25 ° or more and 70 ° or less, and the aspect ratio Str of the surface texture is 0.25 or more and 0.79 or less.
  • Patent Document 2 International Publication No. 2016/117587
  • the average distance between surface peaks on the surface on the release layer side is 20 ⁇ m or less
  • the maximum height difference of the waviness on the surface opposite to the release layer is.
  • a copper foil with a carrier provided with an ultrathin copper foil having a thickness of 1.0 ⁇ m or less is disclosed, and according to such an embodiment, it is said that both fine circuit formability and laser processability can be achieved at the same time.
  • Patent Document 3 Japanese Unexamined Patent Publication No.
  • a copper foil with a carrier having a Sp / Spk ratio of 3.271 or more and 10.739 or less with Spk is disclosed.
  • one of the physical adhesion indexes between the circuit and the substrate is the shear strength, and in order to effectively avoid the above-mentioned circuit peeling, it is required to keep the shear strength above a certain level.
  • the roughened particles of the copper foil must be enlarged, and there is a problem that it is difficult to achieve both etching properties.
  • the present inventors have recently applied a surface profile in a roughened copper foil in which the developed area ratio Sdr of the interface and the level difference Sk of the core portion defined in ISO25178 are controlled within predetermined ranges, respectively. It was found that excellent etching properties and high area strength can be achieved at the same time in the processing of stretched laminated boards or the manufacture of printed wiring boards.
  • an object of the present invention is to provide a roughened copper foil capable of achieving both excellent etching properties and high market share strength in the processing of copper-clad laminates or the production of printed wiring boards.
  • a roughened copper foil having a roughened surface on at least one side.
  • the roughened surface has an interface development area ratio Sdr of 3.50% or more and 12.00 measured under the conditions of a cutoff wavelength of 0.55 ⁇ m by the S filter and a cutoff wavelength of 10 ⁇ m by the L filter in accordance with ISO25178. % Or less, and the level difference Sk of the core portion measured under the conditions of a cutoff wavelength of 0.55 ⁇ m by the S filter and a cutoff wavelength of 10 ⁇ m by the L filter in accordance with ISO25178 is 0.15 ⁇ m or more and 0.35 ⁇ m or less.
  • Roughened copper foil is provided.
  • the carrier, the release layer provided on the carrier, and the roughened copper foil provided on the release layer with the roughened surface facing outward are provided.
  • a copper foil with a carrier is provided.
  • a copper-clad laminate provided with the roughened copper foil is provided.
  • a printed wiring board provided with the roughened copper foil is provided.
  • the “interface development area ratio Sdr” indicates how much the development area (surface area) of the definition region, which is measured in accordance with ISO25178, is increased with respect to the area of the definition region. It is a parameter.
  • the developed area ratio Sdr of the interface is expressed as an increase (%) in the surface area. The smaller this value is, the more flat the surface is, and the Sdr of the completely flat surface is 0%. On the other hand, the larger this value is, the more uneven the surface shape is. For example, a surface Sdr of 40% indicates that the surface has a 40% increase in surface area from a perfectly flat surface.
  • 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 in accordance with ISO25178. say.
  • the load area ratio is a parameter representing the area of a region having a certain height c or more.
  • the load area ratio at height c corresponds to Smr (c) in FIG.
  • the secant line of the load curve drawn from the load area ratio of 0% along the load curve with the difference of the load area ratio set to 40% is moved from the load area ratio of 0%, and the secant line is used.
  • the position where the slope is the gentlest is called the central part of the load curve.
  • the straight line that minimizes the sum of squares of the deviations in the vertical axis direction with respect to this central portion is called an equivalent straight line.
  • the portion included in the height range of the load area ratio of the equivalent straight line from 0% to 100% is called the core portion.
  • the part higher than the core part is called the protruding peak part, and the part lower than the core part is called the protruding valley part.
  • the “core level difference Sk” is a value obtained by subtracting the minimum height from the maximum height of the core portion measured in accordance with ISO25178, and as shown in FIG. It is a parameter calculated by the difference in height between 0% and 100% of the load area ratio of the equivalent straight line.
  • the "maximum height Sz" is a parameter representing the distance from the highest point to the lowest point on the surface, which is measured in accordance with ISO25178.
  • the "surface texture aspect ratio Str” is a parameter representing the isotropic or anisotropy of the surface texture, which is measured in accordance with ISO25178. Str ranges from 0 to 1, and usually shows strong isotropic when Str> 0.5, and conversely shows strong anisotropy when Str ⁇ 0.3.
  • the “peak peak density Spd” is a parameter representing the number of peak peaks per unit area measured in accordance with ISO25178, and is a peak peak larger than 5% of the maximum amplitude in the contour curved surface. Only points shall be counted. A large value suggests that the number of contact points with other objects is large.
  • the interface development area ratio Sdr, the core level difference Sk, the maximum height Sz, the surface aspect ratio Str, and the peak density Spd of the peaks are two-dimensional regions of a predetermined measurement area (for example, 16384 ⁇ m 2) on the roughened surface. ) Can be calculated by measuring the surface profile with a commercially available laser microscope.
  • each numerical value of the developed area ratio Sdr of the interface, the level difference Sk of the core portion, the maximum height Sz, and the aspect ratio Str of the surface texture is the cutoff wavelength of 0.55 ⁇ m by the S filter and the cutoff by the L filter. The value shall be measured under the condition of a wavelength of 10 ⁇ m.
  • the numerical value of the peak density Spd of the peak is a value measured under the conditions of a cutoff wavelength of 3 ⁇ m by the S filter and a cutoff wavelength of 10 ⁇ m by the L filter.
  • the "electrode surface” of the carrier refers to the surface on the side that was in contact with the cathode when the carrier was manufactured.
  • the "precipitation surface" of the carrier refers to the surface on which electrolytic copper is deposited during carrier production, that is, the surface on the side that is not in contact with the cathode.
  • the copper foil according to the present invention is a roughened copper foil.
  • This roughened copper foil has a roughened surface on at least one side.
  • the developed area ratio Sdr of the interface is 3.50% or more and 12.00% or less
  • the level difference Sk of the core portion is 0.15 ⁇ m or more and 0.35 ⁇ m or less.
  • the present inventors roughened by controlling the level difference Sk of the core portion, which is a parameter not including the protruding peak portion, and the developing area ratio Sdr, which is a parameter including the protruding peak portion.
  • Sk the level difference
  • Sdr the developing area ratio
  • the generation of protruding peaks can be suppressed, and each roughened particle constituting the roughened treated surface can be configured to bite into the resin on average, whereby fine particles having excellent etching properties can be formed. It has been found that a roughened copper foil having a bump height and a specific surface area that is convenient for ensuring a high shear strength while being a surface can be obtained.
  • the roughened copper foil preferably has an interface development area ratio Sdr of 3.50% or more and 12.00% or less on the roughened surface. It is 4.50% or more and 8.50% or less, more preferably 4.50% or more and 6.00% or less. Within such a range, a sufficient adhesive area with the resin laminated at the time of manufacturing a copper-clad laminate or a printed wiring board is secured, even though the surface has a fine surface (roughening height) with excellent etching properties. This can improve the circuit adhesion from the viewpoint of share strength.
  • the roughened copper foil has a core level difference Sk of 0.15 ⁇ m or more and 0.35 ⁇ m or less on the roughened surface, preferably 0. It is 23 ⁇ m or more and 0.35 ⁇ m or less, more preferably 0.25 ⁇ m or more and 0.35 ⁇ m or less.
  • Sk core level difference
  • the roughened particles constituting the roughened surface can bite into the resin on average.
  • Adhesion with resin is improved.
  • the unevenness becomes a protruding peak on the roughening treatment surface.
  • unevenness protruding mountain portion
  • the maximum height Sz and the like used in the conventional evaluation are parameters including the protruding peaks. Therefore, when trying to improve the circuit adhesion based on such a parameter, the roughening height tends to be large, and therefore the etching property tends to be lowered.
  • the level difference Sk of the core portion is a parameter that does not include the protruding peak portion as described above. Therefore, by using the level difference Sk of the core portion as an evaluation index, it is possible to accurately obtain the optimum surface shape for improving the adhesion with the resin, and as a result, the increase in the roughening height can be suppressed. Is also possible.
  • the roughened copper foil has a Sk / Sdr of 0.038 or more and 0.050 or less, which is the ratio of the level difference Sk ( ⁇ m) of the core portion to the developed area ratio Sdr (%) of the interface on the roughened surface.
  • Sk / Sdr 0.038 or more and 0.050 or less
  • the uneven shape of the roughened surface has less unevenness in height, and not only the uneven shape of the roughened surface is large (that is, the surface area is large), but also the core.
  • the height of the part can also be sufficiently secured.
  • the level difference Sk of the core portion is a parameter obtained by excluding the protruding peak portion, while the developed area ratio Sdr is a parameter obtained including the protruding peak portion. Therefore, when the number of protruding peaks increases or decreases, the value of the level difference Sk of the core portion is constant, but the value of the developed area ratio Sdr changes. Therefore, by controlling the ratio of the level difference Sk of the core portion and the developed area ratio Sdr within the above range, it is possible to suppress the occurrence of protruding peaks on the roughened surface. It is possible to make it easy for each roughened particle constituting the roughened surface to bite into the resin on average. As a result, excellent etching properties and high share strength can be realized in a more balanced manner.
  • the roughened copper foil preferably has Sz ⁇ Sk, which is the product of the maximum height Sz ( ⁇ m) on the roughened surface and the level difference Sk ( ⁇ m) of the core portion, of 0.25 or more and 0.50 or less. , More preferably 0.36 or more and 0.50 or less. Within such a range, the uneven shape of the roughened surface is more suitable to suppress the occurrence of protruding peaks, and to realize excellent etching property and high share strength in a well-balanced manner. Become. Further, from the viewpoint of realizing a fine surface having more excellent etching property, the roughened surface of the roughened copper foil preferably has a maximum height Sz of 1.6 ⁇ m or less, more preferably 1.0 ⁇ m. It is 1.4 ⁇ m or more, more preferably 1.0 ⁇ m or more and 1.2 ⁇ m or less.
  • the roughened copper foil preferably has a peak density Spd of 2.00 ⁇ 10 4 mm -2 or more and 3.00 ⁇ 10 4 mm -2 or less on the roughened surface, more preferably 2.20. It is ⁇ 10 4 mm ⁇ 2 or more and 3.00 ⁇ 10 4 mm ⁇ 2 or less, more preferably 2.75 ⁇ 10 4 mm ⁇ 2 or more and 2.85 ⁇ 10 4 mm ⁇ 2 or less. By doing so, it is possible to secure a sufficient adhesion point with the resin laminated at the time of manufacturing the copper-clad laminate or the printed wiring board, and it is possible to more effectively improve the circuit adhesion from the viewpoint of the share strength. can.
  • the roughened copper foil preferably has an aspect ratio Str of the surface texture on the roughened surface of 0.2 or more and 0.5 or less, more preferably 0.24 or more and 0.50 or less, and further preferably 0. It is 45 or more and 0.50 or less. Within such a range, there will be undulations on the roughened surface that are convenient for adhesion to the resin. As a result, it is possible to more effectively improve the circuit adhesion from the viewpoint of share strength, even though the surface is fine with excellent etching properties.
  • the thickness of the roughened copper foil is not particularly limited, but is preferably 0.1 ⁇ m or more and 35 ⁇ m or less, more preferably 0.5 ⁇ m or more and 5.0 ⁇ m or less, and further preferably 1.0 ⁇ m or more and 3.0 ⁇ m or less.
  • the roughened copper foil is not limited to the one obtained by roughening the surface of a normal copper foil, and may be a roughened copper foil surface of a copper foil with a carrier.
  • the thickness of the roughened copper foil does not include the height of the roughened particles formed on the surface of the roughened surface (the thickness of the copper foil itself constituting the roughened copper foil). Is.
  • a copper foil having a thickness in the above range may be referred to as an ultrathin copper foil.
  • the roughened copper foil has a roughened surface on at least one side. That is, the roughened copper foil may have roughened surfaces on both sides, or may have roughened surfaces on only one side.
  • the roughened surface is typically provided with a plurality of roughened particles (humps), and it is preferable that each of the plurality of roughened particles is made of copper particles.
  • the copper particles may be made of metallic copper or may be made of a copper alloy.
  • the roughening treatment for forming the roughened surface can be preferably performed by forming roughened particles with copper or a copper alloy on the copper foil.
  • roughening treatment is performed according to a plating method that goes through at least two types of plating steps, including a burn-plating step of depositing and adhering fine copper particles on a copper foil and a covering plating step for preventing the fine copper grains from falling off. Is preferably performed.
  • carboxybenzotriazole (CBTA) is added to a copper sulfate solution containing a copper concentration of 5 g / L or more and 20 g / L or less and a sulfuric acid concentration of 180 g / L or more and 240 g / L or less to a concentration of 20 ppm or more and 29 ppm or less. It was added as a temperature of 15 °C above 35 ° C. or less, preferably performed 14A / dm 2 or more 24A / dm 2 hands electrodeposition below.
  • the cover plating step is performed in a copper sulfate solution containing a copper concentration of 50 g / L or more and 100 g / L or less and a sulfuric acid concentration of 200 g / L or more and 250 g / L or less at a temperature of 40 ° C. or more and 60 ° C. or less at 2 A / dm 2 or more. It is preferable to carry out electrodeposition at 4 A / dm 2 or less.
  • the burn-plating step by adding carboxybenzotriazole within the above concentration range to the plating solution, the occurrence of protruding peaks is suppressed on the roughened surface while maintaining the etching property close to that of pure copper.
  • the roughened particles constituting the roughened surface can be configured to bite into the resin on average, and it becomes easy to form bumps on the treated surface that are convenient for satisfying the above-mentioned surface parameters. Further, in the burn-plating step and the cover-plating step, by performing electrodeposition with a lower current density than in the conventional method, it becomes easier to form more convenient bumps on the treated surface in order to satisfy the above-mentioned surface parameters.
  • the roughened copper foil may be subjected to a rust preventive treatment to form a rust preventive treatment layer.
  • the rust preventive 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, and further preferably 2.7 or more and 4 or less in terms of mass ratio.
  • the rust preventive treatment preferably further includes a chromate treatment, and it is more preferable that the chromate treatment is performed on the surface of the plating containing zinc after the plating treatment using zinc. By doing so, the rust prevention property can be further improved.
  • a particularly preferable rust preventive treatment is a combination of a zinc-nickel alloy plating treatment and a subsequent chromate treatment.
  • the surface of the roughened 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 the silane coupling agent, applying it, and drying it.
  • silane coupling agents include epoxy functional silane coupling agents such as 4-glycidylbutyltrimethoxysilane and 3-glycidoxypropyltrimethoxysilane, or 3-aminopropyltrimethoxysilane, N- (2- (2-).
  • Amino-functional silane coupling agent, or mercapto-functional silane coupling agent such as 3-mercaptopropyltrimethoxysilane, or olefin-functional silane coupling agent such as vinyltrimethoxysilane and vinylphenyltrimethoxysilane, or 3-methacry.
  • acrylic functional silane coupling agents such as loxypropyltrimethoxysilane
  • imidazole functional silane coupling agents such as imidazole silane
  • triazine functional silane coupling agents such as triazinesilane
  • the roughened copper foil preferably further includes a rust preventive treatment layer and / or a silane coupling agent layer on the roughened surface, and more preferably the rust preventive treatment layer and the silane coupling agent layer. It has both.
  • the rust preventive treatment layer and the silane coupling agent layer may be formed not only on the roughened surface side of the roughened copper foil but also on the side where the roughened surface is not formed.
  • the roughened copper foil of the present invention may be provided in the form of a copper foil with a carrier. That is, according to a preferred embodiment of the present invention, the carrier, the release layer provided on the carrier, and the roughening-treated copper foil provided on the release layer with the roughening-treated surface facing outward are provided. Copper foil with a carrier is provided. However, as the copper foil with a carrier, a known layer structure can be adopted except that the roughened copper foil of the present invention is used.
  • the carrier is a support for supporting the roughened copper foil and improving its handleability, and a typical carrier includes a metal layer.
  • a typical carrier includes a metal layer.
  • Examples of such a carrier include aluminum foil, copper foil, stainless steel (SUS) foil, a resin film or glass whose surface is metal-coated with copper or the like, and copper foil is preferable.
  • the copper foil may be either a rolled copper foil or an electrolytic copper foil, but is preferably an electrolytic copper foil.
  • the thickness of the carrier is typically 250 ⁇ m or less, preferably 9 ⁇ m or more and 200 ⁇ m or less.
  • the surface of the carrier on the release layer side is smooth. That is, in the process of manufacturing a copper foil with a carrier, an ultrathin copper foil (before roughening treatment) is formed on the surface of the carrier on the release layer side.
  • the roughened copper foil of the present invention is used in the form of a copper foil with a carrier, the roughened copper foil can be obtained by subjecting such an ultrathin copper foil to a roughening treatment. Therefore, by smoothing the surface of the carrier on the release layer side, the outer surface of the ultrathin copper foil can also be smoothed, and by applying a roughening treatment to the smooth surface of the ultrathin copper foil, the surface can be roughened.
  • the surface of the carrier on the release layer side can be smoothed, for example, by polishing the surface of the cathode used for electrolytic foil forming of the carrier with a buff having a predetermined count to adjust the surface roughness. That is, the surface profile of the cathode thus adjusted is transferred to the electrode surface of the carrier, and the ultrathin copper foil is formed on the electrode surface of the carrier via the release layer, whereby the outer surface of the ultrathin copper foil is formed. It is possible to impart a smooth surface state that facilitates the realization of the roughened surface described above.
  • the preferred buff count is # 2000 or more and # 3000 or less, and more preferably # 2000 or more and # 2500 or less.
  • the peeling layer is a layer having a function of weakening the peeling strength of the carrier, ensuring the stability of the strength, and further suppressing the mutual diffusion that may occur between the carrier and the copper foil during press molding at a high temperature. ..
  • the release layer is generally formed on one surface of the carrier, but may be formed on both sides.
  • the release layer may be either an organic release layer or an inorganic release layer.
  • the organic component used in the organic exfoliation 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, and among them, the triazole compound is preferable because the peelability is easily stable.
  • triazole compounds examples include 1,2,3-benzotriazole, carboxybenzotriazole, N', N'-bis (benzotriazolylmethyl) urea, 1H-1,2,4-triazole and 3-amino-. Examples thereof include 1H-1,2,4-triazole and the like.
  • sulfur-containing organic compounds examples include mercaptobenzothiazole, thiothianulic acid, 2-benzimidazole thiol and the like.
  • carboxylic acids include monocarboxylic acids, dicarboxylic acids and the like.
  • examples of the inorganic component used in the inorganic release layer include Ni, Mo, Co, Cr, Fe, Ti, W, P, Zn, and a chromate-treated film.
  • the release layer may be formed by bringing the release layer component-containing solution into contact with at least one surface of the carrier and fixing the release layer component to the surface of the carrier.
  • this contact may be performed by immersion in the release layer component-containing solution, spraying the release layer component-containing solution, flowing down the release layer component-containing solution, or the like.
  • a method of forming a film of the release layer component by a vapor phase method such as thin film deposition or sputtering can also be adopted.
  • 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 release layer is typically 1 nm or more and 1 ⁇ m or less, preferably 5 nm or more and 500 nm or less.
  • another functional layer may be provided between the release layer and the carrier and / or the roughened copper foil.
  • An example of such another functional layer is an auxiliary metal layer.
  • the auxiliary metal layer is preferably made of nickel and / or cobalt. By forming such an auxiliary metal layer on the surface side of the carrier and / or on the surface side of the roughened copper foil, it may occur between the carrier and the roughened copper foil during hot press molding at a high temperature or for a long time. Mutual diffusion can be suppressed and the stability of the peeling strength of the carrier can be ensured.
  • the thickness of the auxiliary metal layer is preferably 0.001 ⁇ m or more and 3 ⁇ m or less.
  • the roughened copper foil of the present invention is preferably used for producing copper-clad laminates for printed wiring boards. That is, according to a preferred embodiment of the present invention, a copper-clad laminate provided with the roughened copper foil is provided.
  • This copper-clad laminate comprises the roughened copper foil of the present invention and a resin layer provided in close contact with the roughened surface of the roughened copper foil.
  • the roughened copper foil may be provided on one side of the resin layer or may be provided on both sides.
  • the resin layer contains a resin, preferably an insulating resin.
  • the resin layer is preferably a prepreg and / or a resin sheet.
  • Prepreg is a general term for composite materials in which a base material such as a synthetic resin plate, a glass plate, a glass woven fabric, a glass non-woven fabric, or paper is impregnated with a synthetic resin.
  • Preferred examples of the insulating resin include epoxy resin, cyanate resin, bismaleimide triazine resin (BT resin), polyphenylene ether resin, phenol resin and the like.
  • examples of the insulating resin constituting 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 roughened copper foil via a primer resin layer previously applied to the surface of the copper foil.
  • the roughened copper foil of the present invention is preferably used for producing a printed wiring board. That is, according to a preferred embodiment of the present invention, a printed wiring board provided with the roughened copper foil is provided. By using the roughened copper foil of the present invention, it is possible to achieve both excellent etching properties and high market share strength in the production of a printed wiring board.
  • the printed wiring board according to this embodiment includes a layer structure in which a resin layer and a copper layer are laminated.
  • the copper layer is a layer derived from the roughened copper foil of the present invention.
  • the resin layer is as described above for the copper-clad laminate.
  • the printed wiring board can adopt a known layer structure except that the roughened copper foil of the present invention is used.
  • the printed wiring board examples include a single-sided or double-sided printed wiring board in which a circuit is formed by adhering the roughened copper foil of the present invention to one or both sides of a prepreg to form a cured laminate, or a multilayer of these.
  • Examples include a multi-layer printed wiring board.
  • a flexible printed wiring board, COF, TAB tape, etc., in which the roughened copper foil of the present invention is formed on a resin film to form a circuit can be mentioned.
  • a copper foil with resin (RCC) obtained by applying the above-mentioned resin layer to the roughened copper foil of the present invention was formed, and the resin layer was laminated on the above-mentioned printed circuit board as an insulating adhesive layer.
  • the roughened copper foil is used as the whole or part of the wiring layer, and the build-up wiring board in which the circuit is formed by the modified semi-additive (MSAP) method, the subtractive method, etc., and the roughened copper foil are removed.
  • MSAP modified semi-additive
  • Examples thereof include a build-up wiring board in which a circuit is formed by a semi-additive method, and a direct build-up on wafer in which a copper foil with a resin is laminated and a circuit is formed alternately on a semiconductor integrated circuit.
  • Examples thereof include electronic materials for glass, electromagnetic wave shield films obtained by applying a conductive adhesive to the roughened copper foil of the present invention.
  • the roughened copper foil of the present invention is suitable for the MSAP method.
  • the configuration shown in FIGS. 1 and 2 can be adopted.
  • Examples 1-7, 9 and 10 A copper foil with a carrier provided with a roughened copper foil was prepared and evaluated as follows.
  • the electrode surface of the pickled carrier is placed in a CBTA aqueous solution containing a carboxybenzotriazole (CBTA) 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.
  • CBTA carboxybenzotriazole
  • the CBTA component was adsorbed on the electrode surface of the carrier.
  • the CBTA layer was formed as an organic release layer on the electrode surface of the carrier.
  • the carrier on which the organic exfoliation layer is formed is immersed in a solution containing nickel sulfate and having a nickel concentration of 20 g / L, so that the liquid temperature is 45 ° C., pH 3 and the current density is 5 A /. Under the condition of dm 2 , an adhering amount of nickel corresponding to a thickness of 0.001 ⁇ m was adhered on the organic release layer. In this way, a nickel layer was formed as an auxiliary metal layer on the organic release layer.
  • the surface of the ultrathin copper foil thus formed was roughened to form a roughened copper foil, whereby a copper foil with a carrier was obtained.
  • This roughening treatment comprises a burn-plating step of depositing and adhering fine copper particles on an ultrathin copper foil, and a covering plating step for preventing the fine copper grains from falling off.
  • carboxybenzotriazole (CBTA) having a concentration shown in Table 1 is added to an acidic copper sulfate solution containing a copper concentration of 10 g / L and a sulfuric acid concentration of 200 g / L at a liquid temperature of 25 ° C. and shown in Table 1.
  • Roughening treatment was performed at the current density.
  • electrodeposition was performed using an acidic copper sulfate solution containing a copper concentration of 70 g / L and a sulfuric acid concentration of 240 g / L under smooth plating conditions of a liquid temperature of 52 ° C. and a current density shown in Table 1. ..
  • various samples having different roughening-treated surface characteristics were prepared by appropriately changing the CBTA concentration and current density in the burn-plating step and the current density in the cover plating step as shown in Table 1.
  • the surface of the obtained roughened copper foil with a carrier was subjected to a rust prevention treatment consisting of a zinc-nickel alloy plating treatment and a chromate treatment.
  • a rust prevention treatment consisting of a zinc-nickel alloy plating treatment and a chromate treatment.
  • the roughening treatment layer and carriers are used under the conditions of a liquid temperature of 40 ° C. and a current density of 0.5 A / dm 2.
  • the surface of the surface was plated with a zinc-nickel alloy.
  • the surface subjected to the zinc-nickel alloy plating treatment was subjected to chromate treatment under the conditions of pH 12 and a current density of 1 A / dm 2.
  • Silane Coupling Agent Treatment A silane coupling agent treatment is performed by adsorbing a commercially available aqueous solution containing a silane coupling agent on the surface of the copper foil with a carrier to roughen the copper foil side and evaporating the water content with an electric heater. Was done. At this time, the silane coupling agent treatment was not performed on the carrier side.
  • the level difference Sk of the core part and the peak density Spd of the peak were measured.
  • the Sz, Sdr, Str and Sk were measured with the cutoff wavelength of the S filter set to 0.55 ⁇ m and the cutoff wavelength of the L filter set to 10 ⁇ m.
  • the cutoff wavelength by the S filter was set to 3 ⁇ m, and the cutoff wavelength by the L filter was set to 10 ⁇ m. The results were as shown in Table 1.
  • An evaluation laminate was prepared using the obtained copper foil with a carrier. That is, as shown in FIG. 5, roughened copper foil with a carrier is provided on the surface of the insulating resin substrate 111 via a prepreg 112 (GHPL-830NSF, thickness 0.1 mm, manufactured by Mitsubishi Gas Chemical Company, Inc.). The foil 110 was laminated and thermocompression bonded at a pressure of 4.0 MPa and a temperature of 220 ° C. for 90 minutes, and then the carrier (not shown) was peeled off to obtain a copper-clad laminate as the evaluation laminate 114. In the example shown in FIG. 5, the roughened copper foil 110 includes roughened particles 110a on its surface.
  • the required etching amount varies depending on the thickness of the ultrathin copper foil. Therefore, as shown in FIG. 5, the thickness of the roughened copper foil 110 in the evaluation laminate 114 is equivalent to 1.5 ⁇ m (excluding the thickness of the roughened particles 110a) for evaluation.
  • the thickness of the laminate 114 was reduced by half-etching or increased by copper sulfate plating, if necessary.
  • the evaluation laminate 114 whose thickness of the roughened copper foil 110 was adjusted to 1.5 ⁇ m was etched with a sulfuric acid-hydrogen peroxide-based etching solution by 0.1 ⁇ m, and the surface copper (roughened particles 110a) was etched. The amount (depth) until completely disappeared (including) was measured.
  • the measurement was performed by confirming with an optical microscope (500 times). More specifically, the work of confirming the presence or absence of copper with an optical microscope was repeated every time 0.1 ⁇ m was etched, and the value ( ⁇ m) obtained by (number of etchings) ⁇ 0.1 ⁇ m was used as an index of etchability.
  • the measured etching amount was rated and evaluated according to the following criteria, and if it was evaluated as any of A to C, it was judged to be acceptable. The results were as shown in Table 1.
  • the shear strength when the circuit 136 was pushed from the side of the circuit sample for shear strength measurement was measured. That is, as shown in FIG. 6, the laminated body 134 on which the circuit 136 is formed is placed on the movable stage 132, and the stage 132 is moved in the direction of the arrow in the drawing to the detector 138 which is fixed in advance. By pressing the circuit 136, a lateral force was applied to the side surface of the circuit 136 to shift the circuit 136 laterally, and the force (gf) at that time was measured by the detector 138 and adopted as the share strength.
  • a junction strength tester 4000 Plus Bondester manufactured by Nordson DAGE
  • the test type was a fracture test, and the measurement was performed under the conditions of a test height of 5 ⁇ m, a descent speed of 0.050 mm / s, a test speed of 200 ⁇ m / s, a tool movement amount of 0.05 mm, and a fracture recognition point of 10%.
  • the obtained share strength was rated and evaluated according to the following criteria, and if it was evaluated as any of A to C, it was judged to be acceptable. The results were as shown in Table 1.
  • Example 8 (comparison) Copper foils with carriers were prepared and evaluated in the same manner as in Example 1 except for the following a) to c). The results were as shown in Table 1.
  • a) Career preparation was performed according to the procedure shown below.
  • b) Instead of the electrode surface of the carrier, a release layer, an auxiliary metal layer and an ultrathin copper foil were formed on the precipitation surface of the carrier in this order.
  • c) instead of the burnt plating step and the cover plating step, the ultrathin copper foil was roughened by the black plating step shown below.
  • a sulfuric acid acidic copper sulfate solution having the composition shown below was used as the copper electrolytic solution, a titanium electrode having a surface roughness Ra of 0.20 ⁇ m was used as the cathode, and DSA (dimensional stability anode) was used as the anode. Electrolysis was performed at a solution temperature of 45 ° C. and a current density of 55 A / dm 2 , and an electrolytic copper foil having a thickness of 12 ⁇ m was obtained as a carrier.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Laminated Bodies (AREA)
  • Electroplating Methods And Accessories (AREA)
  • Manufacturing Of Printed Wiring (AREA)

Abstract

L'invention fournit une feuille de cuivre traitée par rugosification qui permet de concilier d'excellentes propriétés de gravure et une résistance élevée au cisaillement, lors de l'usinage d'une carte stratifiée cuivrée ou de la fabrication d'une carte de circuit imprimé. Cette feuille de cuivre traitée par rugosification possède une face traitée par rugosification sur au moins un côté. La face traitée par rugosification présente un rapport de surface développée (Sdr) pour une interface, mesuré sous des conditions de longueur d'onde de coupure de ０,５５μｍ par un filtre S et de longueur d'onde de coupure de １０μｍ par un filtre L conformément à ＩＳＯ２５１７８, supérieur ou égal à ３,５０％ et inférieur ou égal à １２,００％. La feuille de cuivre traitée par rugosification de l'invention présente une différence de niveau (Sk) pour une partie noyau, mesurée sous des conditions de longueur d'onde de coupure de ０,５５μｍ par un filtre S et de longueur d'onde de coupure de １０μｍ par un filtre L conformément à ＩＳＯ２５１７８, supérieure ou égale à 0,1５μｍ et inférieure ou égale à ０,３５μｍ.
PCT/JP2021/001902 2020-02-04 2021-01-20 Feuille de cuivre traitée par rugosification, feuille de cuivre avec support, carte stratifiée cuivrée, et carte de circuit imprimé WO2021157362A1 (fr)

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KR1020227022468A KR20220106200A (ko) 2020-02-04 2021-01-20 조화 처리 동박, 캐리어를 구비하는 동박, 동장 적층판 및 프린트 배선판
JP2021575705A JP7259093B2 (ja) 2020-02-04 2021-01-20 粗化処理銅箔、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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WO2022153580A1 (fr) * 2021-01-15 2022-07-21 Ｊｘ金属株式会社 Feuille de cuivre traitée en surface, stratifié cuivré et carte de circuit imprimé
WO2023281759A1 (fr) * 2021-07-09 2023-01-12 Ｊｘ金属株式会社 Feuille de cuivre traitée en surface, stratifié cuivré et carte de circuit imprimé

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WO2023281759A1 (fr) * 2021-07-09 2023-01-12 Ｊｘ金属株式会社 Feuille de cuivre traitée en surface, stratifié cuivré et carte de circuit imprimé

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