WO2011061894A1 - プリプレグ、積層板、金属箔張積層板、回路基板及びled搭載用回路基板 - Google Patents
プリプレグ、積層板、金属箔張積層板、回路基板及びled搭載用回路基板 Download PDFInfo
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- WO2011061894A1 WO2011061894A1 PCT/JP2010/006415 JP2010006415W WO2011061894A1 WO 2011061894 A1 WO2011061894 A1 WO 2011061894A1 JP 2010006415 W JP2010006415 W JP 2010006415W WO 2011061894 A1 WO2011061894 A1 WO 2011061894A1
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- aluminum hydroxide
- prepreg
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
- H05K1/00—Printed circuits
- H05K1/02—Details
- H05K1/03—Use of materials for the substrate
- H05K1/0313—Organic insulating material
- H05K1/0353—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement
- H05K1/0373—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement containing additives, e.g. fillers
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
- C08J5/24—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B15/00—Layered products comprising a layer of metal
- B32B15/14—Layered products comprising a layer of metal next to a fibrous or filamentary layer
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B32B5/00—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts
- B32B5/22—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed
- B32B5/24—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed one layer being a fibrous or filamentary layer
- B32B5/26—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed one layer being a fibrous or filamentary layer another layer next to it also being fibrous or filamentary
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B5/00—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts
- B32B5/22—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed
- B32B5/24—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed one layer being a fibrous or filamentary layer
- B32B5/28—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed one layer being a fibrous or filamentary layer impregnated with or embedded in a plastic substance
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
- C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
- C08G59/20—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the epoxy compounds used
- C08G59/32—Epoxy compounds containing three or more epoxy groups
- C08G59/38—Epoxy compounds containing three or more epoxy groups together with di-epoxy compounds
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- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
- C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
- C08G59/40—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the curing agents used
- C08G59/4007—Curing agents not provided for by the groups C08G59/42 - C08G59/66
- C08G59/4014—Nitrogen containing compounds
- C08G59/4021—Ureas; Thioureas; Guanidines; Dicyandiamides
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- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
- C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
- C08G59/40—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the curing agents used
- C08G59/62—Alcohols or phenols
- C08G59/621—Phenols
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- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
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- C08J5/24—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs
- C08J5/241—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs using inorganic fibres
- C08J5/244—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs using inorganic fibres using glass fibres
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
- C08J5/24—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs
- C08J5/249—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs characterised by the additives used in the prepolymer mixture
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
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- C08K3/01—Use of inorganic substances as compounding ingredients characterized by their specific function
- C08K3/013—Fillers, pigments or reinforcing additives
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- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
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- B32B2260/00—Layered product comprising an impregnated, embedded, or bonded layer wherein the layer comprises an impregnation, embedding, or binder material
- B32B2260/02—Composition of the impregnated, bonded or embedded layer
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- B32B2305/07—Parts immersed or impregnated in a matrix
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
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- C08K2003/2227—Oxides; Hydroxides of metals of aluminium
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
- H05K1/00—Printed circuits
- H05K1/02—Details
- H05K1/03—Use of materials for the substrate
- H05K1/0313—Organic insulating material
- H05K1/0353—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement
- H05K1/0366—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement reinforced, e.g. by fibres, fabrics
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
- H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
- H05K2201/01—Dielectrics
- H05K2201/0104—Properties and characteristics in general
- H05K2201/012—Flame-retardant; Preventing of inflammation
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
- H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
- H05K2201/02—Fillers; Particles; Fibers; Reinforcement materials
- H05K2201/0203—Fillers and particles
- H05K2201/0206—Materials
- H05K2201/0209—Inorganic, non-metallic particles
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
- H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
- H05K2201/02—Fillers; Particles; Fibers; Reinforcement materials
- H05K2201/0203—Fillers and particles
- H05K2201/0263—Details about a collection of particles
- H05K2201/0266—Size distribution
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- 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
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- Y10T428/24802—Discontinuous or differential coating, impregnation or bond [e.g., artwork, printing, retouched photograph, etc.]
- Y10T428/24917—Discontinuous or differential coating, impregnation or bond [e.g., artwork, printing, retouched photograph, etc.] including metal layer
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- 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
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- 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
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- 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
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- 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
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- Y10T442/20—Coated or impregnated woven, knit, or nonwoven fabric which is not [a] associated with another preformed layer or fiber layer or, [b] with respect to woven and knit, characterized, respectively, by a particular or differential weave or knit, wherein the coating or impregnation is neither a foamed material nor a free metal or alloy layer
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Definitions
- the present invention relates to a prepreg used in the field of circuit boards for various electronic devices, and particularly excellent in heat dissipation, and a laminate, a metal foil-clad laminate, a circuit board, and an LED manufactured using the prepreg
- the present invention relates to a circuit board for mounting.
- FR-4 As a typical laminate used for a printed circuit board for electronic equipment, a laminate called FR-4 obtained by laminating a prepreg in which a glass cloth is impregnated with a resin component such as an epoxy resin is used. Widely used.
- the name FR-4 is a classification according to a standard by NEMA (National Electrical Manufactures Association) in the United States.
- NEMA National Electrical Manufactures Association
- a layer in which a nonwoven fabric is impregnated with a resin component is used as a core material layer, and a glass cloth is impregnated with a layer in which a glass cloth is impregnated as a surface layer on each surface of the core material layer.
- a composite laminate called three types is also known.
- Patent Document 1 listed below discloses a resin-impregnated core obtained by impregnating a nonwoven fabric and / or paper with a resin varnish as a composite laminate having high interlaminar adhesive strength and excellent alkali resistance, heat resistance, and punchability.
- a composite laminate is proposed in which a resin-impregnated surface layer material obtained by impregnating a glass cloth with a resin varnish is adhered to both surfaces of a material, and a metal foil is further adhered.
- the resin varnish used for the core contains a filler that combines talc and aluminum hydroxide, and the blending ratio of talc and aluminum hydroxide is 0.15 to 0.65: It is described that aluminum hydroxide is boehmite type.
- Patent Document 2 as a composite laminate having excellent thermal stability and thermal stability, it is composed of a surface layer composed of a resin-impregnated glass woven fabric and an intermediate layer composed of a curable resin-impregnated glass nonwoven fabric. Laminated materials for printed circuit boards have been proposed.
- the intermediate layer has a molecular formula of Al 2 O 3 .nH 2 O (wherein n is greater than 2.6 and in an amount of 200% to 275% by weight based on the resin in the intermediate layer) It contains aluminum hydroxide (having a value less than 2.9).
- the present invention has been made in view of the above-described problems, and an object of the present invention is to provide a laminate having excellent thermal conductivity, heat resistance, drilling workability, and flame retardancy.
- thermosetting resin composition is inorganic with respect to 100 parts by volume of the thermosetting resin.
- the inorganic filler contains 80 to 200 parts by volume of filler, and (A) gibbsite type aluminum hydroxide particles having an average particle diameter (D 50 ) of 2 to 15 ⁇ m, (B) average particle diameter of 2 to 15 ⁇ m A group consisting of boehmite particles having (D 50 ), and inorganic particles having an average particle diameter (D 50 ) of 2 to 15 ⁇ m and containing crystal water having a liberation start temperature of 400 ° C.
- the compounding ratio (volume ratio) of at least one inorganic component (B) selected from the group consisting of yttrium particles and inorganic particles and the aluminum oxide particles (C) is 1: 0.1 to 2.5: 0. . Relates to a laminate of 1 to 1;
- Another aspect of the present invention relates to a metal foil-clad laminate in which a metal foil is stretched on at least one surface of the prepreg, and a circuit board obtained by forming a circuit on the metal foil-clad laminate, and It is related with the circuit board for LED mounting which consists of the said circuit board.
- FIG. 1 is a schematic cross-sectional view of a prepreg according to an embodiment of the present invention.
- FIG. 2 is a schematic configuration diagram of the LED backlight unit.
- the prepreg according to the present invention is obtained by impregnating a woven fabric base material with a thermosetting resin composition.
- thermosetting resin composition A preferred embodiment according to the present invention will be described first for a thermosetting resin composition.
- thermosetting resin composition contains 80 to 200 parts by volume of an inorganic filler with respect to 100 parts by volume of the thermosetting resin, and the inorganic filler contains (A) average particles of 2 to 15 ⁇ m.
- Gibbsite-type aluminum hydroxide particles having a diameter (D 50 )
- B boehmite particles having an average particle diameter (D 50 ) of 2 to 15 ⁇ m
- an average particle diameter (D 50 ) of 2 to 15 ⁇ m At least one inorganic component selected from the group consisting of inorganic particles containing crystal water having a temperature of 400 ° C. or higher or not containing crystal water, and (C) an average particle diameter (D 50 ) of 1.5 ⁇ m or less.
- thermosetting resins include liquid thermosetting resins such as epoxy resins; radical polymerization thermosetting resins such as unsaturated polyester resins and vinyl ester resins; Moreover, a hardening
- the inorganic filler according to the present embodiment includes a group consisting of gibbsite-type aluminum hydroxide particles (A), boehmite particles, and inorganic particles that contain crystal water having a liberation start temperature of 400 ° C. or higher or no crystal water. At least one inorganic component (B) selected from the following and aluminum oxide particles (C).
- the gibbsite-type aluminum hydroxide particles (A) are aluminum compounds represented by Al (OH) 3 or Al 2 O 3 .3H 2 O, and the laminate is thermally conductive, flame retardant, and drillable. Is a component that imparts a good balance.
- the average particle diameter (D 50 ) of the gibbsite type aluminum hydroxide particles (A) is 2 to 15 ⁇ m, preferably 3 to 10 ⁇ m.
- the gibbsite-type aluminum hydroxide particles (A) include a first gibbsite-type aluminum hydroxide having an average particle diameter (D 50 ) of 2 to 10 ⁇ m and a second gibbsite-type aluminum hydroxide particle (D 50 ) of 10 to 15 ⁇ m. It is preferable to use a blend with Gibbsite type aluminum hydroxide from the viewpoint that heat dissipation is further improved by more densely filling the filler.
- the average particle diameter (D 50 ) in this embodiment is obtained by calculating the cumulative curve with the total volume of the powder group obtained by measurement with a laser diffraction particle size distribution measuring device as 100%, and the cumulative curve is 50%. Means the particle diameter of the point.
- the inorganic component (B) is at least one selected from the group consisting of boehmite particles and inorganic particles that contain crystallization water having a freezing start temperature of 400 ° C. or higher or that do not have crystallization water.
- the boehmite particle is an aluminum compound represented by (AlOOH) or (Al 2 O 3 .H 2 O), and imparts thermal conductivity and flame retardancy without reducing the heat resistance of the laminate. It is.
- the average particle size (D 50 ) of the boehmite particles is 2 to 15 ⁇ m, preferably 3 to 10 ⁇ m.
- the average particle diameter (D 50 ) of the boehmite particles exceeds 15 ⁇ m, drill workability decreases, and when it is less than 2 ⁇ m, thermal conductivity decreases and productivity decreases.
- inorganic particles containing crystallization water having a liberation start temperature of 400 ° C. or higher or having no crystallization water are components that impart thermal conductivity and flame retardancy without lowering the heat resistance of the circuit board. .
- the inorganic particles include inorganic oxides such as aluminum oxide (no crystal water), magnesium oxide (no crystal water), crystalline silica (no crystal water); boron nitride (no crystal water), aluminum nitride (crystals) Inorganic nitrides such as silicon nitride (no crystal water); inorganic carbides such as silicon carbide (no crystal water); and talc (freezing start temperature 950 ° C.), calcined kaolin (no crystal water), clay (free Natural minerals such as a starting temperature of 500 to 1000 ° C.). These may be used alone or in combination of two or more. Among these, magnesium oxide is particularly preferable because it is excellent in thermal conductivity and drill wear.
- magnesium oxide is particularly preferable because it is excellent in thermal conductivity and drill wear.
- the freezing start temperature of crystal water can be measured using heating weight loss analysis (TGA) or suggestion scanning calorimetry (DSC).
- TGA heating weight loss analysis
- DSC suggestion scanning calorimetry
- the average particle diameter (D 50 ) of the inorganic particles is 2 to 15 ⁇ m, preferably 3 to 10 ⁇ m. When the average particle diameter (D 50 ) of the inorganic particles exceeds 15 ⁇ m, drill workability may be reduced.
- Aluminum oxide particles (C) are components that impart high thermal conductivity to the resulting prepreg.
- the average particle diameter (D 50 ) of the aluminum oxide particles (C) is 1.5 ⁇ m or less, preferably 0.4 to 0.8 ⁇ m.
- the average particle diameter of the aluminum oxide particles exceeds 1.5 ⁇ m, it becomes difficult to fill the laminated plate with a sufficient blending amount, and drill workability is also lowered.
- the average particle diameter of aluminum oxide is too small, there exists a possibility that the thermal conductivity of a prepreg may become inadequate.
- the mixing ratio (volume ratio) of the gibbsite type aluminum hydroxide particles (A), the inorganic component (B), and the aluminum oxide particles (C) is 1: 0.1 to 2.5: 0.1 to 1, preferably 1: 0.5 to 2.5: 0.1 to 0.5.
- the blending amount of the inorganic component (B) exceeds 2.5 with respect to the blending amount 1 of the gibbsite-type aluminum hydroxide particles (A)
- the drillability and flame retardancy of the resulting laminate are reduced. If it is less than 0.1, the heat resistance is lowered.
- the blending amount of the aluminum oxide particles (C) exceeds 1 with respect to the blending amount 1 of the gibbsite-type aluminum hydroxide particles (A)
- the drill workability is deteriorated. Reduces the thermal conductivity.
- magnesium oxide particles are preferable from the balance of thermal conductivity and drill workability. Further, the magnesium oxide particles preferably have a specific surface area of 0.1 to 1.5 m 2 / g. This is because, if the specific surface area of the magnesium oxide particles is within the above range, there is an advantage that no void is generated even when the inorganic filler is highly filled.
- the blending ratio of the inorganic filler to 100 parts by volume of the thermosetting resin is 80 to 200 parts by volume, preferably 90 to 140 parts by volume, and more preferably 100 to 130 parts by volume.
- the blending ratio of the inorganic filler to 100 parts by volume of the thermosetting resin is preferably 120 parts by volume or more.
- the compounding ratio of the inorganic filler is less than 80 parts by volume, the thermal conductivity of the obtained laminate is low, and when it exceeds 200 parts by volume, the drilling workability is lowered and the laminate Manufacturability (resin impregnation property, moldability) also decreases.
- the blending ratio of the gibbsite type aluminum hydroxide particles (A) is too large, specifically when it exceeds 100 parts by volume, the heat resistance tends to decrease due to the generation of a large amount of crystal water. There is.
- the inorganic component (B) is a mixture of boehmite particles and inorganic particles containing crystal water having a liberation start temperature of 400 ° C. or higher or having no crystal water, compounding of inorganic particles
- the ratio is preferably 50% by volume or less, more preferably 30% by volume or less, and particularly preferably 20% by volume or less in the total amount of the inorganic filler.
- the thermosetting resin composition includes an inorganic filler containing the above-described gibbsite type aluminum hydroxide particles (A), an inorganic component (B), and aluminum oxide particles (C) in a liquid thermosetting resin. It mix
- a prepreg is obtained by impregnating a resin varnish into a woven fiber substrate such as a glass cloth (woven cloth) or a synthetic fiber cloth (woven cloth) using synthetic fibers such as aramid fiber, polyester fiber, and nylon fiber. It is done.
- a resin varnish containing an epoxy resin, a radical polymerization type thermosetting resin such as an unsaturated polyester resin or a vinyl ester resin as a resin component may be used.
- curing agent, and a filler suitably with the resin varnish for forming a prepreg as needed.
- blend a filler suitably as needed in the range which does not impair the effect of this invention.
- thermosetting resin composition contained in the resin varnish to be impregnated into the woven fiber substrate it is preferable to use a thermosetting resin composition containing the following inorganic filler. That is, the inorganic filler contains 80 to 200 parts by volume of inorganic filler relative to 100 parts by volume of the thermosetting resin, and the inorganic filler contains gibbsite-type aluminum hydroxide particles (A 50 ) having an average particle diameter (D 50 ) of 2 to 15 ⁇ m. ), Boehmite particles having an average particle diameter (D 50 ) of 2 to 15 ⁇ m, and water of crystallization having an average particle diameter (D 50 ) of 2 to 15 ⁇ m and a freezing start temperature of 400 ° C.
- gibbsite-type aluminum hydroxide particles A 50
- Boehmite particles having an average particle diameter (D 50 ) of 2 to 15 ⁇ m
- water of crystallization having an average particle diameter (D 50 ) of 2 to 15 ⁇ m and a freezing start temperature of 400 ° C.
- inorganic component (B) selected from the group consisting of inorganic particles not containing crystal water, and aluminum oxide particles (C) having an average particle size (D 50 ) of 1.5 ⁇ m or less, Curing wherein the mixing ratio (volume ratio) of the type aluminum hydroxide particles (A), the inorganic component (B) and the aluminum oxide particles (C) is 1: 0.1 to 2.5: 0.1 to 1 Resin composition It is preferable to use a product.
- the laminated plate 10 generally has a layer configuration in which a plurality of prepregs are laminated and integrated. And the metal foil 3 is laminated
- the prepreg is obtained by impregnating a woven fiber base material 2a such as a glass cloth with a resin composition 2b.
- Each prepreg may be a single sheet or a plurality of sheets, specifically, one to three layers may be stacked, and may be appropriately adjusted according to the purpose.
- metal foil Copper foil, aluminum foil, nickel foil, etc. can be used.
- the metal foil may be disposed on both surfaces or only on one surface. In addition, it may replace with metal foil and may arrange
- gibbsite type aluminum hydroxide particles (A) are blended in the resin composition, and a predetermined amount of aluminum oxide particles (C) having a small average particle size is blended. Therefore, wear of the drill blade during drilling of the laminated plate can be suppressed. Therefore, the life of the drill can be extended. Moreover, even if a drilling process is applied to form a through hole, it is difficult for irregularities to be formed on the inner surface of the hole to be formed, and the inner surface of the hole can be formed smoothly. For this reason, when through-holes are formed by plating the inner surface of the holes, high conduction reliability can be imparted to the through-holes.
- the heat conductivity of a laminated board can be improved remarkably by mix
- blend the aluminum oxide particle (C) of a small particle diameter the drill workability of a laminated board is not reduced remarkably.
- heat conductivity can be provided by mix
- the prepreg excellent in thermal conductivity and drilling workability of this embodiment has high heat dissipation such as a printed wiring board of an LED backlight unit mounted on a liquid crystal display, a printed wiring board of LED lighting, or the like. It is preferably used for required applications.
- an LED backlight unit 20 mounted on a liquid crystal display as shown in the schematic top view of FIG. 2 is configured by arranging a large number of LED modules 23 each having a plurality of (three in FIG. 2) LEDs 22 mounted on a printed wiring board 21, and is disposed on the back of the liquid crystal panel. Therefore, it is used as a backlight for a liquid crystal display or the like.
- a cold cathode tube (CCFL) type backlight has been widely used as a backlight of the liquid crystal display, but in recent years, compared with a cold cathode tube type backlight. Since the color gamut can be widened, the image quality can be improved, the environmental load is small because mercury is not used, and the LED backlight unit as described above can be reduced in thickness. Is being actively developed.
- LED modules generally consume more power than cold cathode tubes, and therefore generate a large amount of heat.
- the composite laminate of the present invention as the printed wiring board 21 that requires such high heat dissipation, the problem of heat dissipation is greatly improved. Therefore, the luminous efficiency of the LED can be improved.
- thermosetting resin composition used in the examples a thermosetting resin composition used in the examples, a phosphorus-containing epoxy resin was prepared as shown below.
- Example 1 Manufacture of prepreg> Gibbsite type aluminum hydroxide (Sumitomo Chemical Co., Ltd.) is used with respect to 100 parts by volume of the thermosetting resin content of the thermosetting resin varnish containing the phosphorus-containing epoxy resin and the dicyandiamide (Dicy) type curing agent prepared by the above method.
- Gibbsite type aluminum hydroxide Suditomo Chemical Co., Ltd.
- the obtained copper foil-clad laminate was evaluated for thermal conductivity, 220 ° C. oven heat resistance test, 260 ° C. solder heat resistance test, pressure cooker test (PCT), drill wear rate, and flame resistance according to the following evaluation methods. .
- the results are shown in Tables 1 and 2 below.
- Tables 1 to 4 below the values shown in parentheses in each example and each comparative example are the blending ratio of boehmite particles, inorganic particles or aluminum oxide particles to 1 part by volume of gibbsite type aluminum hydroxide particles. To express.
- Thermal conductivity After peeling the copper foil of the obtained copper foil-clad laminate, the density of the laminate from which the copper foil was peeled was measured by an underwater substitution method, the specific heat was measured by DSC (differential scanning calorimetry), The thermal diffusivity was measured by the laser flash method.
- Thermal conductivity (W / m ⁇ K) Density (kg / m 3 ) x Specific heat (kJ / kg ⁇ K) x Thermal diffusivity (m 2 / S) x 1000
- PCT Pressure cooker test
- the obtained copper foil-clad laminate was cut into a predetermined size and subjected to a combustion test in accordance with the UL-94 combustion test method for determination.
- Examples 2 to 19 and Comparative Examples 1 to 20 In the production of the core material layer prepreg, a laminate was obtained and evaluated in the same manner as in Example 1 except that the composition of the resin composition was changed as shown in Tables 1 to 4. The results of Example 1 and Examples 2 to 19 are shown in Tables 1 and 2, and the results of Comparative Examples 1 to 20 are shown in Tables 3 to 4.
- the materials used in the examples and comparative examples are as follows. -(B1) Talc with an average particle size (D 50 ) of 5.5 ⁇ m (manufactured by Fuji Talc Industrial Co., Ltd.) ⁇ (B2) average particle size (D 50) crystalline silica ⁇ (B4) of 6.5 [mu] m average particle diameter (D 50) 6.5 [mu] m, magnesium oxide having a specific surface area (BET) 1.0m 2 / g ⁇ (B5 ) Aluminum nitride with an average particle size (D 50 ) of 6.6 ⁇ m (Furukawa Electronics) (B6) Magnesium oxide having an average particle diameter (D 50 ) of 5 ⁇ m and specific surface area (BET) of 2.5 m 2 / g Aluminum oxide particles having an average particle diameter (D 50 ) of 4 ⁇ m (manufactured by Sumitomo Chemical Co., Ltd.)
- the thermal conductivity was as high as 1.2 (W / (m ⁇ K)) or more. Heat resistance was also excellent in all tests. The drill wear rate was also 65% or less. The flame retardancy was also at the V-0 level.
- Example 18 it was found that by including magnesium oxide as the inorganic component (B), a laminate having a good balance of high thermal conductivity, high heat resistance, and low drill wear rate can be obtained.
- Example 19 it was also found that when magnesium oxide having a high specific surface area was included, there was a problem that voids were generated in the laminate.
- thermosetting resin When only the inorganic filler 70 was contained with respect to 100 parts by volume of the thermosetting resin (Comparative Example 19), the thermal conductivity was low and the flame retardancy was at the V-1 level. Further, when the blending ratio of talc (inorganic component B) to 1 part by volume of gibbsite-type aluminum hydroxide exceeds 2.5 (Comparative Example 20), the flame retardancy was at the V-1 level.
- one aspect of the present invention is a prepreg in which a woven fabric substrate is impregnated with a thermosetting resin composition, and the thermosetting resin composition is contained in 100 parts by volume of the thermosetting resin.
- the inorganic filler contains 80 to 200 parts by volume of the inorganic filler.
- the free starting temperature contains water of crystallization is 400 ° C.
- inorganic particles containing no crystal water At least one inorganic component selected from the group consisting of: and (C) aluminum oxide particles having an average particle diameter (D 50 ) of 1.5 ⁇ m or less, and the gibbsite type aluminum hydroxide particles (A)
- the blending ratio (volume ratio) of at least one inorganic component (B) selected from the group consisting of boehmite particles and inorganic particles and the aluminum oxide particles (C) is 1: 0.1 to 2.5. : 0.1 to 1 laminate.
- a laminate having excellent thermal conductivity, heat resistance, drill workability, and flame retardancy can be obtained.
- thermal conductivity drilling workability will fall remarkably when a general aluminum oxide is mix
- the heat resistance is remarkably improved without reducing drill workability.
- Gibbsite-type aluminum hydroxide (Al (OH) 3 or Al 2 O 3 .3H 2 O), which is an aluminum compound, is a component that imparts heat conductivity, drill workability, and flame retardancy in a well-balanced manner.
- Gibbsite type aluminum hydroxide has a characteristic of releasing crystal water at about 200 to 230 ° C., and therefore has a particularly high effect of imparting flame retardancy.
- it becomes a cause of generating a blister etc. at the time of solder reflow.
- boehmite which is an aluminum-based compound, contributes to imparting thermal conductivity and heat resistance to the laminate.
- Boehmite is potentially superior in heat resistance to gibbsite type aluminum hydroxide because it has the potential to release crystal water at about 450-500 ° C. In addition, it exhibits flame retardancy at high temperatures.
- inorganic particles containing crystallization water having a release start temperature of 400 ° C. or higher or not containing crystallization water similarly contribute to imparting thermal conductivity and heat resistance to the laminate.
- By blending such inorganic particles it is possible to suppress the occurrence of blisters during reflow soldering of the circuit board.
- the flame retardance at the time of high temperature can also be exhibited.
- thermosetting resin composition A laminate obtained using such a thermosetting resin composition is preferably used for various substrates that require high heat dissipation, particularly for LED mounting substrates on which a plurality of LEDs that generate a large amount of heat are mounted. Can be.
- a printed wiring board made of such a laminated board is surface-mounted with various electronic components, blisters are hardly generated on the metal foil even at a temperature of about 260 ° C., which is a lead-free reflow soldering temperature.
- the gibbsite type aluminum hydroxide particles (A) has a first gibbsite type aluminum hydroxide having an average particle size of 2 ⁇ 10 ⁇ m (D 50), the average particle size of 10 ⁇ 15 [mu] m to (D 50) A blend with the second gibbsite type aluminum hydroxide is preferred.
- the laminated board especially excellent in heat conductivity is obtained by being more closely filled with an inorganic filler.
- Examples of the inorganic particles that are one of the inorganic components (B) include aluminum oxide, magnesium oxide, crystalline silica, aluminum hydroxide, boron nitride, aluminum nitride, silicon nitride, silicon carbide, talc, calcined kaolin, and clay. At least one kind of particles selected from the group consisting of
- a surface layer obtained by impregnating a woven fiber base material with a thermosetting resin composition in which the same components as the thermosetting resin composition described above are blended in the same composition ratio is the core material layer.
- a laminate obtained by laminating and integrating the both surfaces is preferable. According to the said structure, the laminated board which has the outstanding heat conductivity, the outstanding heat resistance, the outstanding drill workability, and a flame retardance is obtained.
- a circuit board obtained from such a laminate is excellent in heat dissipation, flame retardancy, and particularly drillability. Therefore, it can be preferably used as a circuit board on which electronic components such as LEDs that require heat dissipation are mounted.
- a laminated board and a circuit board excellent in all of thermal conductivity, heat resistance, drill workability, and flame retardancy can be obtained.
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Abstract
Description
本発明に係る好ましい実施形態を、先ず、熱硬化性樹脂組成物について説明する。
本発明の一実施形態に係る積層板10について、図1を参照しながら説明する。
攪拌装置、温度計、冷却管、窒素ガス導入装置を備えた4つ口のガラス製セパラブルフラスコに、HCA 130重量部、と反応溶媒としてキシレン400重量部を仕込み、加熱して溶解した。その後、1,4-ナフトキノン94重量部、を反応熱による昇温に注意しながら分割投入した。このときリン化合物であるHCAは1,4-ナフトキノン1モルに対して1.02モルであった。反応後、溶媒を300重量部回収した後、EPPN-501H(三官能エポキシ樹脂、エポキシ当量:165g/eq、日本化薬株式会社製)350重量部とエポトート ZX-1355(1,4-ジヒドロキシナフタレン型エポキシ樹脂、エポキシ当量:145g/eq、東都化成株式会社製)250重量部、エポトート YDF-170(ビスフェノールF型エポキシ樹脂、エポキシ当量:168g/eq、東都化成株式会社製)176重量部を仕込み、窒素ガスを導入しながら加熱攪拌を行って更に溶媒を回収した。触媒としてトリフェニルホスフィンを0.22重量部添加して160℃で4時間反応した。得られたエポキシ樹脂は42.6重量%で、エポキシ当量は273.5g/eq、リン含有率は1.85重量%であった。
〈プリプレグの製造〉
上記の方法により調製されたリン含有エポキシ樹脂とジシアンジアミド(Dicy)系硬化剤とを含有する熱硬化性樹脂ワニスの熱硬化性樹脂分100体積部に対して、ギブサイト型水酸化アルミニウム(住友化学(株)製、D50:5.4μm)35体積部、ギブサイト型水酸化アルミニウム(住友化学(株)製、D50:12.6μm)35体積部、ベーマイト(D50:5.5μm)15体積部、及び酸化アルミニウム(住友化学(株)製、D50:0.76μm)15体積部を配合し、均一に分散させた。充填材が配合された樹脂ワニスを、目付け47g/m2、厚み53μmのガラスクロス(日東紡社製)に含浸させプリプレグを得た。そのときのクロス体積は12体積%であった。
得られた銅箔張積層板の銅箔を剥離したのち、銅箔を剥離した積層体の密度を水中置換法により測定し、また、比熱をDSC(示差走査熱量測定)により測定し、さらに、レーザーフラッシュ法により熱拡散率を測定した。
熱伝導率(W/m・K)=密度(kg/m3)×比熱(kJ/kg・K)×熱拡散率(m2/S)×1000
得られた銅箔張積層板を用いて、JIS C 6481に準じて作製した試験片を220℃に設定した空気循環装置付き恒温槽中で一時間処理したときに、銅箔および積層板にふくれ及びはがれが生じなかったときを「優」、ふくれまたははがれが生じたときを「劣」と判定した。
得られた銅箔張積層板を用いて、JIS C 6481に準じて作製した試験片を260℃のハンダ浴に浸漬したときに、銅箔および積層板にふくれまたははがれが生じなかったときの最大時間を特定した。
得られた銅箔張積層板を用いて、JIS C 6481に準じて作製した試験片を、121℃、2気圧のオートクレーブ中で60分間処理した。そして、処理された積層板を、260℃のはんだ槽にディッピングしたときに、銅箔および積層板にふくれまたははがれが生じなかったときの最大時間を特定した。
得られた積層体を2枚重ね、ドリル(ドリル径0.3mm)にて160000回転/minで孔を1000個穿設した後のドリルの刃の摩耗率を、ドリル加工前のドリル刃の大きさ(面積)に対するドリル加工により摩耗したドリル刃の(面積)の割合(百分率)により評価した。
得られた銅箔張積層板を所定の大きさに切り出し、UL-94の燃焼試験法に準じて燃焼試験を行い、判定した。
芯材層プリプレグの製造において、樹脂組成物の組成を表1~表4のように変更した以外は実施例1と同様にして積層体を得、評価した。実施例1および実施例2~19の結果を表1~2に、及び比較例1~20の結果を表3~4に示す。
・(B1)平均粒子径(D50)5.5μmのタルク(富士タルク工業社製)
・(B2)平均粒子径(D50)6.5μmの結晶性シリカ
・(B4)平均粒子径(D50)6.5μm、比表面積(BET)1.0m2/gの酸化マグネシウム
・(B5)平均粒子径(D50)6.6μmの窒化アルミニウム(古河電子社製)
・(B6)平均粒子径(D50)5μm、比表面積(BET)2.5m2/gの酸化マグネシウム
・平均粒子径(D50)4μmの酸化アルミニウム粒子(住友化学社製)
Claims (8)
- 織布基材に熱硬化性樹脂組成物を含浸させて得られたプリプレグであって、
前記熱硬化性樹脂組成物は、熱硬化性樹脂100体積部に対して無機充填材80~200体積部を含有し、
前記無機充填材は、(A)2~15μmの平均粒子径(D50)を有するギブサイト型水酸化アルミニウム粒子、(B)2~15μmの平均粒子径(D50)を有するベーマイト粒子、及び2~15μmの平均粒子径(D50)を有する、遊離開始温度が400℃以上である結晶水を含有する、又は結晶水を含有しない無機粒子からなる群から選ばれる少なくとも1種の無機成分、及び(C)1.5μm以下の平均粒子径(D50)を有する酸化アルミニウム粒子を含有し、
前記ギブサイト型水酸化アルミニウム粒子(A)と前記ベーマイト粒子及び前記無機粒子からなる群から選ばれる少なくとも1種の無機成分(B)と前記酸化アルミニウム粒子(C)との配合比(体積比)が、1:0.1~2.5:0.1~1であるプリプレグ。 - 前記ギブサイト型水酸化アルミニウム粒子(A)が、2~10μmの平均粒子径(D50)を有する第1のギブサイト型水酸化アルミニウムと、10~15μmの平均粒子径(D50)を有する第2のギブサイト型水酸化アルミニウムとの配合物である請求項1に記載のプリプレグ。
- 前記無機成分(B)の1種である無機粒子が、酸化アルミニウム、酸化マグネシウム、結晶性シリカ、水酸化アルミニウム、窒化ホウ素、窒化アルミニウム、窒化ケイ素、炭化ケイ素、タルク、焼成カオリン、及びクレーからなる群から選ばれる少なくとも1種の粒子である請求項1または2に記載のプリプレグ。
- 前記無機成分(B)が酸化マグネシウムであることを特徴とする、請求項1~3のいずれかに記載のプリプレグ。
- 前記酸化マグネシウムの比表面積が、0.1~1.5m2/gであることを特徴とする、請求項1~4のいずれかに記載のプリプレグ。
- 請求項1~5の何れか1項に記載のプリプレグの少なくとも一表面に、金属箔が張られてなる金属箔張積層板。
- 請求項6に記載の金属箔張積層板に回路形成して得られる回路基板。
- 請求項7に記載の回路基板からなるLED搭載用回路基板。
Priority Applications (5)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
EP10831294.3A EP2502956B1 (en) | 2009-11-20 | 2010-10-29 | Prepreg, laminate, metal-foil-clad laminate, circuit board, and circuit board for led mounting |
US13/510,770 US8603624B2 (en) | 2009-11-20 | 2010-10-29 | Prepreg, laminate, metal clad laminate, circuit board, and circuit board for LED mounting |
KR1020127013810A KR101718178B1 (ko) | 2009-11-20 | 2010-10-29 | 프리프레그, 적층판, 금속박 피복 적층판, 회로 기판 및 led 탑재용 회로 기판 |
JP2011541796A JP5776019B2 (ja) | 2009-11-20 | 2010-10-29 | プリプレグ、積層板、金属箔張積層板、回路基板及びled搭載用回路基板 |
CN201080052228.5A CN102725334B (zh) | 2009-11-20 | 2010-10-29 | 半固化片、层压板、覆金属箔层压板、电路基板及led搭载用电路基板 |
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JP2009-265440 | 2009-11-20 | ||
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US (1) | US8603624B2 (ja) |
EP (1) | EP2502956B1 (ja) |
JP (1) | JP5776019B2 (ja) |
KR (1) | KR101718178B1 (ja) |
CN (1) | CN102725334B (ja) |
TW (1) | TWI457241B (ja) |
WO (1) | WO2011061894A1 (ja) |
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JP2016003260A (ja) * | 2014-06-16 | 2016-01-12 | パナソニックIpマネジメント株式会社 | プリント配線板用樹脂組成物、プリント配線板用プリプレグ、積層板、金属張積層板、プリント配線板、及び酸化マグネシウム |
JP2016513741A (ja) * | 2013-03-08 | 2016-05-16 | アルケマ フランス | 繊維性基材を含浸するための液体(メタ)アクリルシロップ、繊維性基材を含浸するための方法、及びこのプレ含浸基材の重合後に製造された複合材料 |
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JP6074883B2 (ja) * | 2010-10-29 | 2017-02-08 | パナソニックIpマネジメント株式会社 | プリプレグ、積層板、金属箔張積層板、回路基板及びledモジュール |
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Also Published As
Publication number | Publication date |
---|---|
CN102725334B (zh) | 2014-11-26 |
KR101718178B1 (ko) | 2017-03-20 |
KR20120095938A (ko) | 2012-08-29 |
JP5776019B2 (ja) | 2015-09-09 |
US8603624B2 (en) | 2013-12-10 |
TWI457241B (zh) | 2014-10-21 |
EP2502956B1 (en) | 2017-09-20 |
US20120228010A1 (en) | 2012-09-13 |
EP2502956A4 (en) | 2015-01-21 |
EP2502956A1 (en) | 2012-09-26 |
CN102725334A (zh) | 2012-10-10 |
JPWO2011061894A1 (ja) | 2013-04-04 |
TW201134670A (en) | 2011-10-16 |
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