TWI300380B - - Google Patents

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TWI300380B
TWI300380B TW094124580A TW94124580A TWI300380B TW I300380 B TWI300380 B TW I300380B TW 094124580 A TW094124580 A TW 094124580A TW 94124580 A TW94124580 A TW 94124580A TW I300380 B TWI300380 B TW I300380B
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Taiwan
Prior art keywords
layer
alloy
tungsten
molybdenum
copper foil
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TW094124580A
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English (en)
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TW200609109A (en
Inventor
Yuushi Sato
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Nippon Denkai Ltd
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Publication of TW200609109A publication Critical patent/TW200609109A/zh
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Publication of TWI300380B publication Critical patent/TWI300380B/zh

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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
    • C25D7/00—Electroplating characterised by the article coated
    • C25D7/06—Wires; Strips; Foils
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C28/00—Coating for obtaining at least two superposed coatings either by methods not provided for in a single one of groups C23C2/00 - C23C26/00 or by combinations of methods provided for in subclasses C23C and C25C or C25D
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C28/00—Coating for obtaining at least two superposed coatings either by methods not provided for in a single one of groups C23C2/00 - C23C26/00 or by combinations of methods provided for in subclasses C23C and C25C or C25D
    • C23C28/02—Coating for obtaining at least two superposed coatings either by methods not provided for in a single one of groups C23C2/00 - C23C26/00 or by combinations of methods provided for in subclasses C23C and C25C or C25D only coatings only including layers of metallic material
    • C23C28/023—Coating for obtaining at least two superposed coatings either by methods not provided for in a single one of groups C23C2/00 - C23C26/00 or by combinations of methods provided for in subclasses C23C and C25C or C25D only coatings only including layers of metallic material only coatings of metal elements only
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C28/00—Coating for obtaining at least two superposed coatings either by methods not provided for in a single one of groups C23C2/00 - C23C26/00 or by combinations of methods provided for in subclasses C23C and C25C or C25D
    • C23C28/30—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer
    • C23C28/32—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one pure metallic layer
    • C23C28/321—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one pure metallic layer with at least one metal alloy layer
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C28/00—Coating for obtaining at least two superposed coatings either by methods not provided for in a single one of groups C23C2/00 - C23C26/00 or by combinations of methods provided for in subclasses C23C and C25C or C25D
    • C23C28/30—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer
    • C23C28/32—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one pure metallic layer
    • C23C28/322—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one pure metallic layer only coatings of metal elements only
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C28/00—Coating for obtaining at least two superposed coatings either by methods not provided for in a single one of groups C23C2/00 - C23C26/00 or by combinations of methods provided for in subclasses C23C and C25C or C25D
    • C23C28/30—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer
    • C23C28/34—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates
    • C23C28/345—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates with at least one oxide layer
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C28/00—Coating for obtaining at least two superposed coatings either by methods not provided for in a single one of groups C23C2/00 - C23C26/00 or by combinations of methods provided for in subclasses C23C and C25C or C25D
    • C23C28/30—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer
    • C23C28/34—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates
    • C23C28/345—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates with at least one oxide layer
    • C23C28/3455—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates with at least one oxide layer with a refractory ceramic layer, e.g. refractory metal oxide, ZrO2, rare earth oxides or a thermal barrier system comprising at least one refractory oxide layer
    • 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
    • C25D3/00—Electroplating: Baths therefor
    • C25D3/02—Electroplating: Baths therefor from solutions
    • C25D3/56—Electroplating: Baths therefor from solutions of alloys
    • C25D3/562—Electroplating: Baths therefor from solutions of alloys containing more than 50% by weight of iron or nickel or cobalt
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25D—PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
    • C25D5/00—Electroplating characterised by the process; Pretreatment or after-treatment of workpieces
    • C25D5/10—Electroplating with more than one layer of the same or of different metals
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25D—PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
    • C25D5/00—Electroplating characterised by the process; Pretreatment or after-treatment of workpieces
    • C25D5/60—Electroplating characterised by the structure or texture of the layers
    • C25D5/615—Microstructure of the layers, e.g. mixed structure
    • C25D5/617—Crystalline layers
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25D—PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
    • C25D9/00—Electrolytic coating other than with metals
    • C25D9/04—Electrolytic coating other than with metals with inorganic materials
    • C25D9/08—Electrolytic coating other than with metals with inorganic materials by cathodic processes
    • 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
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25D—PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
    • C25D3/00—Electroplating: Baths therefor
    • C25D3/02—Electroplating: Baths therefor from solutions
    • C25D3/38—Electroplating: Baths therefor from solutions of copper
    • 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
    • C25D5/18—Electroplating using modulated, pulsed or reversing current
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/12—All metal or with adjacent metals
    • Y10T428/12431—Foil or filament smaller than 6 mils
    • Y10T428/12438—Composite
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/12—All metal or with adjacent metals
    • Y10T428/12458—All metal or with adjacent metals having composition, density, or hardness gradient
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/12—All metal or with adjacent metals
    • Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
    • Y10T428/12535—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.] with additional, spatially distinct nonmetal component
    • Y10T428/12583—Component contains compound of adjacent metal
    • Y10T428/1259—Oxide
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/12—All metal or with adjacent metals
    • Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
    • Y10T428/12535—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.] with additional, spatially distinct nonmetal component
    • Y10T428/12611—Oxide-containing component
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/12—All metal or with adjacent metals
    • Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
    • Y10T428/12771—Transition metal-base component
    • Y10T428/12806—Refractory [Group IVB, VB, or VIB] metal-base component
    • Y10T428/12826—Group VIB metal-base component
    • Y10T428/12833—Alternative to or next to each other
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/12—All metal or with adjacent metals
    • Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
    • Y10T428/12771—Transition metal-base component
    • Y10T428/12861—Group VIII or IB metal-base component
    • Y10T428/12903—Cu-base component

Description

1300380 (1) 九、發明說明 r 【發明所屬之技術領域】 本發明係關於用於製造印刷配線板之複合銅箔，係支 撐物金屬層和薄銅層間之剝離強度之穩定優異之複合銅 箔。 【先前技術】
由支撐物金屬層和剝離層和薄銅層所成之附支撐物銅 箔，係被使用於超高密印刷配線板之製造步驟。將附支撐 物銅箔和樹脂基材，層合成型於薄銅層使其面對樹脂基材 後，剝離支撐物金屬層，將薄銅層蝕刻加工形成電路。較 之使用無支撐物金屬層之一般的銅箔時，因得薄化薄銅層 之厚度，有利於微細電路之形成。 作爲剝離層一般性係使用含有苯并三唑系之有機化合 物或鉻氧化合物等之無機化合物之層，但因於高溫剝離層 內之銅擴散，很難自薄銅層剝離支撐物金屬層。因此，建 議支撐物金屬層或薄銅層之一者，面對剝離層之表面形成 防止銅擴散之層（如參照專利文獻1)。 藉由防止銅之擴散，得抑制高溫下之剝離強度之上 昇，但伴隨者層結構之複雜化，被認爲起因於熱膨脹係數 之不同或結晶構造之變化等界面破壞，支撐物金屬層自薄 銅層自發性地剝離，因薄銅層表面之高溫空氣之氧化劣 化，切斷加工時之損傷等，產生損及對作業性或貼銅層合 板之品質不良影響之問題點。 -4- (2) 1300380 專利文獻1 :特開2002-2927 8 8號公報 【發明內容】 〔發明之揭示〕 本發明之目的係提供提高支撐物金屬層和 之剝離強度之穩定性之複合銅箔。 〔用以解決課題之手段〕 本發明係由支撐物金屬層和剝離層和薄銅 之複合銅箔，最主要特徵爲剝離層一側之表面 金或鉬之合金爲主所成，另一側之表面以由含 氧化物或含有鉬之金屬氧化物爲主所成者。如 由鎢之合金或鉬之合金爲主所成之表面中氧/ 原子數比以0.01〜0.99爲宜，較佳爲0.10〜0. 有鎢之金屬氧化物或含有鉬之金屬氧化物爲主 中氧/金屬比，以原子數比以1.0〜9.0爲宜， 〜4.0 〇 主要由含有鎢之金屬氧化物或含有鉬之金 成之表面，以將薄銅層和支撐物金屬層可剝離 使其黏合，一側主要由鎢之合金或鉬之合金爲 面，銅原子於薄銅層和支撐物金屬層之間相互 熱擴散，防止薄銅層和支撐物金屬層之間之黏 成不可剝離。剝離層內以不存在於明確之界面 即組成物爲傾斜性變化爲宜。藉此所成，起因 薄銅箔層間
層三層所成 以由鎢之合 有鎢之金屬 於剝離層以 金屬比，以 60，以由含 所成之表面 較佳爲1 .5 屬氧化物所 程度之強度 主所成之表 地剝離層內 合力增加形 ，以連續性 於熱膨脹係 -5- 1300380
數之不同或結晶構造之變化之應力縮小，不產生自發性地 剝離現象。作爲如此之剝離層，例舉如由鎢之合金和含有 鎢之金屬氧化物所成，鎢之合金之含有率，自由鎢之合金 爲主所成之表面朝向自含有鎢之金屬氧化物爲主所成之表 面連續性減少，含有鎢之金屬氧化物之含有率，自由含有 鎢之金屬氧化物爲主所成之表面朝向由鎢之合金爲主所成
之表面連續性減少。另外一例，例舉由鉬之合金和含有鉬 之金屬氧化物所成，鉬之合金之含有率，自由鉬之合金爲 主所成之表面朝向自含有鉬之金屬氧化物爲主所成之表面 連續性減少，含有鉬之金屬氧化物之含有率，自由以含有 鉬之金屬氧化物爲主所成之表面朝向以鉬之合金爲主所成 之表面連續性減少之剝離層。具有如此剝離層之複合銅 箔，如依照本發明之方法，於支撐物金屬層，將剝離層和 薄銅層藉由電鑛依序形成之複合銅箔之製造方法，作爲使 用於剝離層形成之電解液，得藉由使用鎢酸化合物或鉬酸 化合物，和含有鐵族元素之化合物，和含有檸檬酸之電解 液製造。 〔發明效果〕 本發明之複合銅箔，因無產生高溫下減少剝離強度上 昇，且支撐物金屬層自薄銅層自發性地剝離，致使作業性 或貼銅層合板之品質不良影響等之問題點，具有適於高密 度印刷配線板製造之優點。 1300380
〔用以實施發明之最佳型態〕 本發明所用之支撐物金屬層之材質、厚度並無特別規 定，但以成本或製造步驟、機械特性及化學特性之觀點， 以厚度8//m〜35//m之銅范爲宜。對於表面粗度，若須 具有和薄銅層和樹脂基材之接合強度，支撐物金屬層之表 面粗度以大者爲宜，反之，若須形成微細電路，表面粗度 以小者爲宜。又以薄銅層薄且表面粗度小者爲宜。
剝離層形成前，將支撐物金屬層之表面藉由適當之前 處理加以清淨化爲宜，除通常之酸洗處理外，亦可進行鹼 脫脂或電解洗淨。
本發明之剝離層，得藉由使用含有鎢酸化合物或鉬酸 化合物，和含有鐵族元素之化合物，和檸檬酸之電解液， 將支撐物金屬層作爲陰極進行電鍍形成。作爲鐵族元素以 使用鎳爲宜。電解液以調整電阻値爲目的亦可添加硫酸鈉 等無機鹽。鎢酸化合物或鉬酸化合物之添加量，分別以金 屬換算，通常爲 〇·1〜10g/l，以0.5〜2g/l爲宜。 又，對於含有鐵族元素之化合物，以金屬換算，通常爲 0.6〜60g/l，以3〜12g/l爲宜。檸檬酸之濃度，對於 除鈉離子以外之金屬種以莫耳換算，即鎢酸化合物和含有 鐵族元素化合物之總莫耳數，或對於鉬酸化合物和含有鐵 族元素化合物之總莫耳數，通常爲0.2〜5倍，較佳爲0.5 〜2倍。作爲鎢酸化合物，如得使用鎢酸鈉二水合物等鎢 酸鹽或該水合物。作爲鉬酸化合物，如得使用鉬酸鈉二水 合物等鉬酸鹽或該水合物。作爲含有鐵族元素化合物，如 1300380
得使用硫酸鎳六水合物等鎳鹽或該水合物。作爲檸檬酸 源，如得使用檸檬酸鈉二水合物等檸檬酸鹽或該水合物。 電解液之溶劑通常爲水。電解液溫度通常爲5〜70 °C，以 10〜50 °C爲宜。電流密度通常爲0.2〜10A / dm2，以0.5 〜5A/dm2爲宜。又pH通常爲2〜8，以4〜7之範圍爲 宜。若以上述條件進行電鍍，首先以析出金屬爲主，與電 鍍進行之同時以析出氧化物爲宜。以氧化物爲主體之表面 顯現剝離功能，另方面，以金屬爲主體之表面抑制藉銅原 子之熱擴散之層結構之一體化。剝離層之厚度和組成，依 電解液之組成和電解條件加以控制。通常剝離層之厚度爲 0.005 〜0.5/zmo 剝離層得以一步形成，亦可複數反複電鍍形成。可於 單一槽進行複數電鑛，亦得於複數槽進行電鍍。若以複數 次進行剝離層之形成，剝離強度更加穩定。
薄銅層之形成並無特別限度，但因使用以吡咯啉酸銅 爲主體之電解液形成緻密鍍銅層，氣孔減少。又，若使用 以硫酸銅爲主體之電解液，因可高速電鍍，得較有效率形 成薄銅層。藉組合兩者之電鍍方法，得較有效率形成具有 所期之厚度，氣孔小之薄銅層。薄銅層之厚度可按照用途 隨意設定。爲形成微細電路通常以0.1〜10//m爲宜，但 亦可較厚。又若以此方法製造本發明之複合銅箔，連接於 薄銅層之剝離層之表面，因以氧化物爲主體故剝離強度 小，剝離層殘留於支撐物金屬層側。 薄銅層之表面，可用習知之方法，以提昇和樹脂基材 -8- 1300380
之黏著性爲目的進行粗化處理，亦可藉由鉻鹽酸處理等習 知之方法進行防鏽處理。又，按照需要以提昇和樹脂基材 之黏著性爲目的，亦可藉由有機矽烷偶合劑等進行黏著強 化處理。
利用該本發明之製造方法所製造之複合銅箔，鎢之合 金係含有鎢及鐵族元素之合金，鉬之合金係含有鉬及鐵族 元素之合金，含有鎢之金屬氧化物係含有鎢之氧化物及鐵 族元素之氧化物者，含有鉬之金屬氧化物係含有鉬之氧化 物及鐵族元素之氧化物者。 得將本發明之複合銅箔和樹脂基材，層合成型於複合 銅箔之薄銅層側使其面對樹脂基材作成貼銅層合板，使用 於印刷配線之製造。又，亦得於本發明之複合銅箔之薄銅 層上塗佈樹脂基材溶液，藉由加熱成貼銅樹脂薄膜，使用 於印刷配線板之製造。製造印刷配線板之際，得藉由自貼 銅層合板或貼銅樹脂薄膜剝離支撐物金屬層及剝離層後， 將薄銅層蝕刻加工形成電路，得到印刷配線板。作爲樹脂 基材，如得使用至少含有聚醯亞胺系樹脂、環氧系樹脂、 馬來酸酐縮亞胺系樹脂、三嗪系樹脂、聚苯醚系樹脂、聚 丁二烯系樹脂之任一種。作爲聚醯亞胺系樹脂，例舉如聚 醯亞胺、聚醯胺亞胺，或該等之前驅物質、如聚醯胺酸 等。於貼銅層合板之製造，通常將此類樹脂之至少1種浸 漬於玻璃布之預漬體作爲樹脂基材之用。於貼銅樹脂薄膜 之製造，通常使用含有該樹脂之至少1種之樹脂基材溶 液。 -9- (7) 1300380 【實施方式】 實施例 於支撐物金屬層，使用厚度之電解銅范。將 此銅箔之表面於硫酸中進行陰極處理，將表面清淨化。接 著，將該已清淨化之銅箔作爲陰極以（陽極：鈦基體氧化 銦塗覆電極）表1所載之條件（電解液之p Η ·· 6 · 〇、液溫：
3 (TC )，於光澤面形成剝離層1。又，剝離層1之形成， 於實施例2，以表1所載之條件將銅箔進行2 0秒鐘之陰 極處理後，停止電流，以1 〇秒鐘之間隔，再以20秒鐘相 同之條件進行陰極處理。 剝離層1形成後，依序使用鍍脯氨酸銅浴和鍍硫酸銅 浴形成3.9 // m之薄銅層。用以形成薄銅層之電鑛條件如 下述。 鑛脯氨酸銅 電解液組成：脯氨酸銅80g/ 1、脯氨酸鉀320 g/ 氣水2 m 1 / 1 pH ： 8.5 電流密度·· 2.0A/ dm2、 時間；20秒 溫度：4〇°C 鍍硫酸銅 電解液組成：硫酸銅200g/ 1、硫酸100 g/ 1 -10- 1300380
電流密度：3.5A/dm2、 時間；300秒
溫度：40°C
再用習知之方法進行相當於厚度1 // m之微細粗化， 接著藉由進行鉻酸鹽處理和有機矽烷偶合劑處理，製造複 合銅箔A〜D。又，爲用以比較，除將依序形成剝離層2 和剝離層3代替剝離層1之外，同於複合銅箔A〜D，製 造複合銅箔E。 自複合銅箔A〜E剝離薄銅層，將支撐物金屬層上之 剝離層之表面於深度方向以氬離子蝕刻之同時進行XPS 分析。結果倂示於表1。但氧原子和金屬原子之比，係扣 除銅金屬所算出。複合銅箔A〜D皆於蝕刻初期檢測出氧 多，和蝕刻進行之同時並觀察氧之減少。得知於蝕刻初期 被觀察之面，即連接於薄銅層側之表面，存在以鉬或鎢爲 主之氧化物，連接於支撐物金屬層之面存有金屬。 藉由自無加熱狀態之複合銅箔A〜E剝離薄銅層，將 支撐物金屬層和薄銅層間之剝離強度依據JIS C648 1測 定，結果示於表1。於玻璃布基材環氧樹脂預漬體（相當 於FR — 5)，層合複合銅箔A〜E之薄銅層使其面對基材， 以260°C、30 kN/m2沖壓60分鐘，作成貼銅層合板。 又，於複合銅箔A〜E塗佈市售之聚醯胺酸溶液，以120 °C 1〇〇分鐘，再以200 °C乾燥20分鐘後，以400°C加熱10 分鐘醯亞胺化，作成貼銅聚醯亞胺樹脂薄膜。將支撐物金 屬層和薄銅層間之剝離強度依據JIS C648 1之測定結果示 -11 - (9) 1300380 於表1。表1中，「260°c , ' 製造時沖壓時之加熱條件， 銅聚醯亞胺樹脂薄膜製造時 使用複合銅箔E之貼銅 屬層自發性地剝離，薄銅層 合銅箔A〜D之貼銅聚醯亞j / m2之剝離強度，剝離後: 光澤和金屬銅特有之色相。 60分」其意指該貼銅層合板 「450°C / 10分」其意指該貼 醯亞胺時之加熱條件。 聚醯亞胺樹脂薄膜，支撐物金 之表氧化變色。反之，使用複 安樹脂薄膜，具有20〜280 kN 匕薄銅層表面呈現通常之金屬
-12- (10)1300380 [表l]
實施例1 實施例2 實施例3 實施例4 比較例1 銅范A 銅箔B 銅箔c 銅箔D 銅箔E 浴組成 NiS04 · 6H20 30 30 30 30 — (g/〇 Na2Mo〇4 · 2H2O 3 3 3 — — 剝離層 Na2W04 · 2H20 — 一 — 3 — 1 Na3C6H507 · 2H20 30 30 30 30 — Na2S04 30 30 30 30 — 電流密度（A/dm2) 3 3 3 3 — 電解時間（秒） 40 20+20 20 20 — 浴組成 NiS04 · 6H20 _ — — — 300 (g/1) H3BO3 — 一 _ —— 40 剝離層 H3PO3 _ 一 _ — 0.5 2 MgS04· 6H20 — — — — 80 糖精鈉 2 電流密度（A/dm2) 一 — — — 5.4 電解時間（秒） — 一 — — 20 剝離層 浴組成 Na2Mo〇7 · 2H2O — 一 一 一 2 3 (g/1) Ν&2〇Γ2〇7 · 2H2〇 — 一 — — 2 電流密度（A/dm2) — 一 — — 5.4 電解時間（秒） — — — — 20 剝離強度 無加熱 20 20 20 10 20 (N/m) 260°C /60 分 20 20 20 10 20 4 450°C /10 分 90 20 160 280 自然剝離 剝離層中之酸1 關：〇秒 3.6 3.3 3.3 3.4 5.8 素/金屬（原子1 勤刻：3 0秒 1.6 0.9 1.2 1.2 0.1 數比） 1 i虫刻：6 0秒 0.9 0.8 0.7 0.8 0.1 1 i虫刻：120秒 0.6 0.6 0.6 0.6 0.0 1 1虫刻：2 4 0秒 0.5 0.5 0.5 0.5 0 -13- (11) 1300380 〔產業上之可利用性〕 本發明之複合銅箔，因無產生高溫下減少剝離強度之 上昇，且支撐物金屬層和薄銅層，加工中自發性之剝離， 致使作業性或貼銅層合板之品質不良影響等之問題點，適 於高密度印刷配線板之製造。
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Claims (1)

  1. (1) 1300380 十、申請專利範圍 1· 一種複合銅箔，係由支撐物金屬層，和支撐物金屬 層上之剝離層，和剝離層上之薄銅層三層所成之複合銅 箔，其特徵爲：剝離層一側之表面以鎢之合金或鉬之合金 爲主所成，另一側之表面以含有鎢之金屬氧化物或含有鉬 之金屬氧化物爲主所成者。
    2·如申請專利範圍第1項之複合銅箔，其中支撐物金 屬層爲銅箔。 3 ·如申請專利範圍第1項之複合銅箔，其中鎢之合金 係含有鎢及鐵族元素之合金，鉬之合金係含有鉬及鐵族元 素之合金，含有鎢之金屬氧化物係含有鎢之氧化物及鐵族 元素氧化物者，含有鉬之金屬氧化物係含有鉬之氧化物及 鐵族元素氧化物者。 4·如申請專利範圍第3項之複合銅箱，其中鐵族元素 爲鎳。 5 ·如申請專利範圍第1項之複合銅箔，其中由以鎢之 合金或鉬之合金爲主所成之表面，係連接於支撐物金屬層 之表面，由以含有鎢之金屬氧化物或含有鉬之金屬氧化物 爲主所成之表面，係連接於薄銅層之表面。 6 ·如申請專利範圍第1項之複合銅箔，其中剝離層， 係由鎢之合金和含有鎢之金屬氧化物所成，鎢之合金之含 有率，係自以鎢之合金爲主所成之表面朝向以含有鎢之金 屬氧化爲主所成之表面連續性減少，含有鎢之金屬氧化物 之含有率，係自以含有鎢之金屬氧化物爲主所成之表面朝 -15- (2) 1300380 向以鎢之合金爲主所成之表面連續性減少者。 7·如申請專利範圍第1項之複合銅箔，其中剝離層， 係由鉬之合金和含有鉬之金屬氧化物所成，鉬合金之含有 率，係自以鉬合金爲主所成之表面朝向以含有鉬之金屬氧 化爲主所成之表面連續性減少，含有鉬之金屬氧化物之含 有率，係自以含有鉬之金屬氧化物爲主所成之表面朝向以 鉬合金爲主所成之表面連續性減少者。
    8 · —種如申請專利範圍第1項的複合銅箔之製造方 法，其爲於支撐物金屬層上，將剝離層和薄銅層藉由電鍍 依序形成之複合銅箔之製造法，其特徵爲：作爲剝離層形 成所用之電解液，係使用含有鎢酸化合物或鉬酸化合物， 和含有鐵族元素之化合物，和檸檬酸之電解液者。 9. 如申請專利範圍第8項之複合銅箔之製造方法，其 中支撐物金屬層爲銅箔，鐵族元素爲鎳。 10. —種印刷配線板之製造方法，其特徵爲：係使用 申請專利範圍第1項之複合銅箔和樹脂基材，使複合銅箔 之薄銅層面對樹脂基材進行層合成型之貼銅層合板。 1 1 .如申請專利範圍第1 0項之印刷配線板之製造方 法，其中樹脂基材係至少含有聚醯亞胺系樹脂、環氧系樹 脂、馬來酸酐縮亞胺系樹脂、三嗪系樹脂、聚苯醚系樹 脂、聚丁二烯系樹脂之任一種。 1 2 . —種印刷配線板之製造方法，其特徵爲：係使用 於申請專利範圍第1項之複合銅箔之薄銅層上塗佈樹脂基 材溶液，藉由加熱所得之貼銅樹脂薄膜。 -16- (3) 1300380 1 3 .如申請專利範圍第1 2項之印刷配線板之製造方 法，其中樹脂基材係至少含有聚醯亞胺系樹脂、環氧系樹 脂、馬來酸酐縮亞胺系樹脂、三嗪系樹脂、聚苯醚系樹 脂、聚丁二烯系樹脂之任一種。
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CN1993501A (zh) 2007-07-04
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US7816015B2 (en) 2010-10-19
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MY140573A (en) 2009-12-31
JPWO2006013735A1 (ja) 2008-07-31
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