WO2013118752A1 - Couche de fermeture, carte de circuit imprimé à équiper d'un élément électroluminescent et dispositif formant source d'éclairage - Google Patents

Couche de fermeture, carte de circuit imprimé à équiper d'un élément électroluminescent et dispositif formant source d'éclairage Download PDF

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Publication number
WO2013118752A1
WO2013118752A1 PCT/JP2013/052685 JP2013052685W WO2013118752A1 WO 2013118752 A1 WO2013118752 A1 WO 2013118752A1 JP 2013052685 W JP2013052685 W JP 2013052685W WO 2013118752 A1 WO2013118752 A1 WO 2013118752A1
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Prior art keywords
resin layer
reflectance
coverlay film
wavelength
inorganic filler
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PCT/JP2013/052685
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English (en)
Japanese (ja)
Inventor
純 松井
秀次 鈴木
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三菱樹脂株式会社
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Application filed by 三菱樹脂株式会社 filed Critical 三菱樹脂株式会社
Priority to KR1020147024910A priority Critical patent/KR20140130161A/ko
Priority to JP2013557536A priority patent/JP5676785B2/ja
Priority to CN201380004632.9A priority patent/CN104025726A/zh
Publication of WO2013118752A1 publication Critical patent/WO2013118752A1/fr

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    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
    • C09D183/00—Coating compositions based on macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon, with or without sulfur, nitrogen, oxygen, or carbon only; Coating compositions based on derivatives of such polymers
    • C09D183/04—Polysiloxanes
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L83/00—Compositions of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon only; Compositions of derivatives of such polymers
    • C08L83/04—Polysiloxanes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/48—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor body packages
    • H01L33/58—Optical field-shaping elements
    • H01L33/60—Reflective elements
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K3/00—Apparatus or processes for manufacturing printed circuits
    • H05K3/22—Secondary treatment of printed circuits
    • H05K3/28—Applying non-metallic protective coatings
    • 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
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
    • C08K3/20—Oxides; Hydroxides
    • C08K3/22—Oxides; Hydroxides of metals
    • C08K2003/2237—Oxides; Hydroxides of metals of titanium
    • C08K2003/2241—Titanium dioxide
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2224/00—Indexing scheme for arrangements for connecting or disconnecting semiconductor or solid-state bodies and methods related thereto as covered by H01L24/00
    • H01L2224/01—Means for bonding being attached to, or being formed on, the surface to be connected, e.g. chip-to-package, die-attach, "first-level" interconnects; Manufacturing methods related thereto
    • H01L2224/42—Wire connectors; Manufacturing methods related thereto
    • H01L2224/44—Structure, shape, material or disposition of the wire connectors prior to the connecting process
    • H01L2224/45—Structure, shape, material or disposition of the wire connectors prior to the connecting process of an individual wire connector
    • H01L2224/45001—Core members of the connector
    • H01L2224/45099—Material
    • H01L2224/451—Material with a principal constituent of the material being a metal or a metalloid, e.g. boron (B), silicon (Si), germanium (Ge), arsenic (As), antimony (Sb), tellurium (Te) and polonium (Po), and alloys thereof
    • H01L2224/45138—Material with a principal constituent of the material being a metal or a metalloid, e.g. boron (B), silicon (Si), germanium (Ge), arsenic (As), antimony (Sb), tellurium (Te) and polonium (Po), and alloys thereof the principal constituent melting at a temperature of greater than or equal to 950°C and less than 1550°C
    • H01L2224/45144—Gold (Au) as principal constituent
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2224/00—Indexing scheme for arrangements for connecting or disconnecting semiconductor or solid-state bodies and methods related thereto as covered by H01L24/00
    • H01L2224/01—Means for bonding being attached to, or being formed on, the surface to be connected, e.g. chip-to-package, die-attach, "first-level" interconnects; Manufacturing methods related thereto
    • H01L2224/42—Wire connectors; Manufacturing methods related thereto
    • H01L2224/47—Structure, shape, material or disposition of the wire connectors after the connecting process
    • H01L2224/48—Structure, shape, material or disposition of the wire connectors after the connecting process of an individual wire connector
    • H01L2224/4805—Shape
    • H01L2224/4809—Loop shape
    • H01L2224/48091—Arched
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2224/00—Indexing scheme for arrangements for connecting or disconnecting semiconductor or solid-state bodies and methods related thereto as covered by H01L24/00
    • H01L2224/73—Means for bonding being of different types provided for in two or more of groups H01L2224/10, H01L2224/18, H01L2224/26, H01L2224/34, H01L2224/42, H01L2224/50, H01L2224/63, H01L2224/71
    • H01L2224/732—Location after the connecting process
    • H01L2224/73251—Location after the connecting process on different surfaces
    • H01L2224/73265—Layer and wire connectors
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L33/48—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor body packages
    • H01L33/62—Arrangements for conducting electric current to or from the semiconductor body, e.g. lead-frames, wire-bonds or solder balls
    • 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
    • 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
    • H05K2201/20—Details of printed circuits not provided for in H05K2201/01 - H05K2201/10
    • H05K2201/2054—Light-reflecting surface, e.g. conductors, substrates, coatings, dielectrics

Definitions

  • the present invention protects the surface of a printed wiring board, in particular, a substrate on which a light emitting element such as an LED is mounted.
  • the present invention relates to a substrate and a light source device. More specifically, it has a high reflectivity, and even after passing through a high-temperature heat load environment or a light resistance test environment, a decrease in reflectivity is suppressed, that is, a high reflectivity is maintained, and the phosphor is dispersed.
  • the present invention relates to a coverlay film that can also be used as a dam material when filling resin.
  • Chip type LEDs with LEDs mounted directly on the printed circuit board pattern and resin-sealed are advantageous for miniaturization and thinning. Therefore, electronic devices such as numeric keypad lighting for mobile phones and backlights for small liquid crystal displays are available. Widely used in equipment.
  • the technology for increasing the brightness of LEDs has been remarkably improved, and LEDs have become more bright.
  • the amount of heat generated by the LED element itself increases, and the ambient temperature of the LED element may exceed 100 ° C., which increases the thermal load on components such as a printed wiring board.
  • the heating temperature reaches about 260-300 ° C in the thermosetting process of the sealing resin and the reflow process after joining with lead (Pb) -free solder. The surroundings are exposed to a high temperature heat environment not only during use but also in the manufacturing process.
  • thermosetting resin compositions that have been used in the past, such as thermosetting resin compositions that are coated with a thermosetting solder resist, are used in an environment where a thermal load is applied as described above.
  • a tendency was observed in which the whiteness decreased and the reflection efficiency decreased due to yellowing of the solder resist and the printed wiring board. Therefore, when developing a substrate for mounting a next-generation high-brightness LED in the future, it is necessary to improve such a decrease in reflection efficiency.
  • the degree of whiteness is also the same as in the heat load environment, even in an environment where ultraviolet rays are irradiated. There was a tendency for the reflectivity to decrease due to a decrease.
  • a substrate made of ceramic is excellent in heat resistance, it has a hard and brittle property, so there is a limit to increase the area and thickness. Therefore, there is a possibility that a substrate made of the ceramic may be difficult to be used as a substrate used in future general lighting applications or display applications. Therefore, there has been a demand for the development of a printed wiring board in which a cover lay film is laminated as a heat-resistant substrate that does not cause discoloration or a decrease in reflectance even under a high temperature heat load and can cope with a large area. .
  • the mounting part is filled with a sealing resin (silicone resin, epoxy resin, or the like) in which a phosphor is dispersed.
  • a dam material made of a thermosetting resin for example, a silicone resin or an epoxy resin is formed so that the sealing resin does not leak to the peripheral portion.
  • a dam material is generally formed by a dispenser or the like and thermally cured.
  • the resin when the resin is heat-cured, the wiring portion may be contaminated and the wire bonding property may be affected, or the white solder resist and the printed wiring board material may be thermally deteriorated, so a dam material is formed. It was a challenge.
  • the manufacturing cost is high, development of a coverlay film in which a conductor protective layer such as metal wiring and a dam material are integrated, and a printed wiring board formed by laminating such a coverlay film have been demanded.
  • Patent Document 1 had insufficient initial reflectance and light discoloration resistance. Moreover, there was no description or suggestion about a technology that can be widely applied, such as being usable as a dam material.
  • the object of the present invention is a cover lay film that has high reflectivity in the visible light region, high heat resistance, and low decrease in reflectivity under high-temperature heat load environments and light-proof environments, and can cope with an increase in area.
  • it is to provide a coverlay film that can be used for a printed wiring board for LED mounting, and a light-emitting element mounting substrate and a light source device formed by laminating the coverlay film.
  • polyorganosiloxane was used as a thermosetting resin, and a resin composition containing this resin and an inorganic filler was used as a gamma ray or the like.
  • a resin composition containing this resin and an inorganic filler was used as a gamma ray or the like.
  • the first invention in the present invention includes a resin layer containing a polyorganosiloxane and an inorganic filler, has an average reflectance of 85% or more at a wavelength of 400 to 800 nm, and is at 260 ° C. for 10 minutes. It is a coverlay film for protecting a conductor circuit of a printed wiring board having a reflectance reduction rate at a wavelength of 450 nm after heat treatment of 5% or less.
  • the reflectance reduction rate at a wavelength of 450 nm after the light resistance test shown below is 5% or less.
  • Light resistance test Using a xenon weather meter, irradiation was performed at a temperature of 63 ° C. (black panel temperature), humidity of 50%, and irradiance (295 to 400 nm) of 60 W / m 2 for 50 hours.
  • the resin layer is preferably cured by radiation.
  • the inorganic filler is preferably titanium oxide.
  • the coverlay film preferably has a thickness of 30 to 500 ⁇ m.
  • the average reflectance at a wavelength of 350 to 400 nm is preferably 40% or more.
  • the resin layer (A), a polyorganosiloxane, and a resin layer (B) containing an inorganic filler different from the inorganic filler contained in the resin layer (A) are provided. It is preferable that At this time, the inorganic filler contained in the resin layer (B) is preferably alumina.
  • a protective layer having a resin layer (A) containing a polyorganosiloxane and an inorganic filler is formed on a substrate used for mounting at least one light emitting element.
  • the protective layer has an average reflectance of 85% or more at a wavelength of 400 to 800 nm, and a reduction rate of the reflectance at a wavelength of 450 nm after heat treatment at 260 ° C. for 10 minutes is 5% or less. It is the board
  • a conductor circuit is formed on a substrate, a protective layer is laminated on the conductor circuit, and the light emitting element on the substrate is mounted so that the conductor circuit and the light emitting element are electrically connected.
  • a light source device having a configuration in which the light emitting element is sealed with a resin.
  • the protective layer includes a resin layer (A) containing a polyorganosiloxane and an inorganic filler, has an average reflectance of 85% or more at a wavelength of 400 to 800 nm, and is heat-treated at 260 ° C. for 10 minutes. After that, the light source device is characterized in that the reflectance reduction rate at a wavelength of 450 nm is 5% or less.
  • the cover lay film of the present invention has a high reflectivity not only in the visible light region but also in the ultraviolet region, high heat resistance, and little reduction in reflectivity under high temperature heat load environment and light resistance test environment. Can be obtained. Therefore, the coverlay film of the present invention is useful as a coverlay film for protecting a conductor circuit of a printed wiring board. And the light emitting element mounting substrate and light source device in which the conductor circuit protective layer was formed can be manufactured by using the coverlay film of this invention.
  • the cover lay film according to the first embodiment of the present invention includes a resin layer (A) containing a polyorganosiloxane and an inorganic filler, and has a wavelength of 400 to 800 nm.
  • a coverlay film for protecting a conductor circuit of a printed wiring board having an average reflectance of 85% or more and a reduction rate of reflectance at a wavelength of 450 nm after heat treatment at 260 ° C. for 10 minutes is 5% or less.
  • the coverlay film needs to have an average reflectance of 85% or more at a wavelength of 400 to 800 nm. This is because the higher the reflectance in the visible light region, the higher the luminance of the LED mounted on the substrate, and if it is in the above range, it can be suitably used as a coverlay film for the LED mounting substrate. is there. From this viewpoint, the average reflectance is preferably 90% or more, particularly 95% or more.
  • the reflectance at 450 nm is more preferably 85% or more, particularly 90% or more. In particular, it is preferably 95% or more.
  • the coverlay film may reflect both light having a wavelength of 350 to 400 nm and light having a wavelength in the visible light region (400 to 800 nm), corresponding to the emission wavelength of the ultraviolet (near ultraviolet) LED. It becomes necessary. Therefore, this cover lay film preferably has an average reflectance of 350 to 400 nm of 40% or more, more preferably 60% or more, and particularly preferably 80% or more.
  • polyorganosiloxane As a method for increasing the average reflectance at a wavelength of 400 to 800 nm, the reflectance at 450 nm, and the reflectance at a wavelength in the ultraviolet (near ultraviolet) region (350 to 400 nm) to a predetermined range, polyorganosiloxane An inorganic filler is contained in the resin layer (A) to form a resin layer (A), thereby obtaining extremely excellent reflection characteristics, and a method of appropriately adjusting the type and content of the inorganic filler to be used.
  • This cover lay film requires that the reflectance reduction rate at a wavelength of 450 nm after heat treatment at 260 ° C. for 10 minutes is 5% or less of the reflectance before the heat treatment.
  • thermosetting process 100 to 200 ° C, several hours
  • a sealing agent such as a conductive adhesive, epoxy or silicone resin, soldering process (Pb-free solder reflow, peak temperature 260 ° C)
  • soldering process Pb-free solder reflow, peak temperature 260 ° C
  • a high thermal load such as a wire bonding process.
  • the thermal load on the substrate tends to increase, and the LED element ambient temperature may exceed 100 ° C. Therefore, in the future, it will be important to maintain a high reflectance without discoloration even under such a high heat load environment.
  • wavelength 450nm is an average wavelength of blue LED.
  • the reflectance decrease rate at a wavelength of 450 nm after heat treatment at 260 ° C. for 10 minutes is 5% or less of the reflectance before the heat treatment, it is possible to suppress the decrease in reflectance in the manufacturing process.
  • the rate of decrease is preferably 4% or less, more preferably 3% or less, and particularly preferably 2% or less.
  • this cover-lay film has the reflectance decreasing rate after the next light resistance test of 5% or less of the reflectance before the light resistance test.
  • Light resistance test Irradiated with a xenon weather meter at a temperature of 63 ° C. (black panel temperature), a humidity of 50%, and an irradiance (295 to 400 nm) of 60 W / m 2 for 50 hours.
  • the reflectance decrease rate after the light resistance test is 5% or less of the reflectance before the light resistance test, it is possible to suppress the decrease in reflectance during actual use. It can be suitably used for a mounting substrate. From this viewpoint, the rate of decrease is preferably 4% or less, more preferably 3% or less, and particularly preferably 2% or less.
  • polyorganosiloxane in order to make the reduction rate of the reflectance after heat treatment and the reduction rate of the reflectance after the light resistance test within a desired range, when forming the resin layer (A), polyorganosiloxane
  • the resin composition containing the inorganic filler is preferably cured by radiation, particularly by gamma rays, as will be described later. However, it is not limited to this method.
  • This coverlay film is provided with a resin layer (A) containing a polyorganosiloxane and an inorganic filler.
  • polyorganosiloxane used in the cover lay film are substances having a siloxane skeleton described in formula (1) and capable of causing a crosslinking reaction.
  • polyorganosiloxane There is no restriction
  • R in formula (1) represents an alkyl group such as a methyl group or an ethyl group, a hydrocarbon group such as a vinyl group or a phenyl group, or a halogen-substituted hydrocarbon group such as a fluoroalkyl group.
  • polydimethylsiloxane in which “R” in formula (1) is all methyl groups, or a part of the methyl groups of polydimethylsiloxane is one or more of the above hydrocarbon groups or halogen-substituted hydrocarbon groups.
  • various polyorganosiloxanes substituted by As polyorganosiloxane used for this coverlay film, said polydimethylsiloxane and various polyalkylsiloxane can be used individually or in mixture of 2 or more types.
  • the polyorganosiloxane resin When forming the resin layer (A), the polyorganosiloxane resin may be cured.
  • the curing means for the polyorganosiloxane may be determined by appropriately selecting from any conventionally known methods such as addition type, condensation type, peroxide curing type and the like.
  • condensation type examples include dealcoholization, deacetic acid, deoxime, and dehydrogenation types. Among these, it is preferable to use an addition type polyorganosiloxane that does not generate a by-product during curing.
  • Examples of the method for curing the polyorganosiloxane include a method of adding a curing catalyst, a method of heating at a high temperature, a method of adding a crosslinking agent, and a crosslinking method by irradiation with radiation.
  • Examples of the curing catalyst include aminosilane-based, nickel salt-based, and ammonium salt-based catalysts.
  • metal soaps, such as octylate and naphthenate, such as Al, Fe, Co, Mn, and Zn, platinum catalyst, etc. are mentioned.
  • the condition is generally 150 ° C. to 250 ° C. and can be cured by heating for about 30 minutes to 2 hours.
  • the heating temperature can be lowered.
  • the heating temperature can be set to 100 ° C. to 180 ° C., for example.
  • the heating time can also be shortened to about 10 to 30 minutes, for example, which is preferable.
  • Curing by radiation is a method in which heat is not applied to the polyorganosiloxane, and there is no fear of impairing the heat resistance and light resistance reliability due to the residue of the crosslinking material, and the effect of the present invention becomes remarkable. preferable.
  • examples of the radiation used for curing the polyorganosiloxane include electron beam, X-ray, and ⁇ -ray. These radiations are widely used industrially, can be easily used, and are energy efficient. Among these, it is preferable to use ⁇ rays having little absorption loss and high permeability.
  • the polyorganosiloxane is cured by irradiating the uncrosslinked polyorganosiloxane with, for example, ⁇ rays. Since the crosslinking reaction can be advanced by irradiation with ⁇ rays, the crosslinking reaction can be caused without using a crosslinking agent.
  • the irradiation dose of ⁇ rays may be appropriately selected and determined depending on the resin type, the amount of crosslinking groups, and the type of radiation source, but is generally 10 to 150 kGy. Of these, 20 to 100 kGy is preferable, and 30 to 60 kGy is particularly preferable.
  • the crystalline polyester resin is generally a substrate excellent in resistance to radiation and suitable for the process film of the present invention.
  • Inorganic filler used for resin layer (A) There is no restriction
  • the inorganic filler used in the resin layer (A) is further coated with a silicone compound or a polyhydric alcohol based on the surface of the inorganic filler in order to improve dispersibility in the resin layer (A) made of polyorganosiloxane.
  • a silicone compound or a polyhydric alcohol based on the surface of the inorganic filler in order to improve dispersibility in the resin layer (A) made of polyorganosiloxane.
  • a silicone compound, an amine compound, a fatty acid, a fatty acid ester or the like can be used. Of these, those treated with silicone compounds (such as siloxane and silane coupling agents) are preferred.
  • the inorganic filler used for the resin layer (A) it is preferable to use a material having a large refractive index difference from the polyorganosiloxane in consideration of the light reflectivity of the present coverlay film.
  • those having a refractive index of 1.6 or more are preferable, and specifically, for example, among those described above, calcium carbonate, barium sulfate, zinc oxide, titanium oxide, titanate and the like can be mentioned, and titanium oxide is particularly preferable.
  • Alumina is preferred from the viewpoint of increasing the reflectance in the low wavelength region.
  • Titanium oxide has a significantly higher refractive index than other inorganic fillers, and can increase the difference in refractive index from polyorganosiloxane as the base resin, so it is less than when other fillers are used. It is preferable because excellent reflectivity can be obtained by the blending amount.
  • a crystalline titanium oxide such as anatase type or rutile type is preferable, and in particular, from the viewpoint of increasing the difference in refractive index from the polyorganosiloxane, Rutile type titanium oxide is preferred.
  • the coverlay film is also ultraviolet (nearly near). It is necessary to reflect light with a wavelength of 350 to 400 nm corresponding to the emission wavelength of the ultraviolet LED and to reflect light with a wavelength in the visible light region (400 to 800 nm).
  • the anatase type with less light absorption is preferred.
  • the production method of titanium oxide generally includes a chlorine method and a sulfuric acid method, but as the production method of titanium oxide used in the present invention, it is preferable to use titanium oxide produced by the chlorine method from the viewpoint of whiteness. .
  • the titanium oxide is preferably one whose surface is coated with an inert inorganic oxide.
  • an inert inorganic oxide By coating the surface of titanium oxide with an inert inorganic oxide, the photocatalytic activity of titanium oxide can be suppressed, and deterioration of the coverlay film of the present invention can be suppressed, which is preferable.
  • the inert inorganic oxide specifically, for example, at least one selected from the group consisting of silica, alumina, and zirconia is preferably used. Use of these inert inorganic oxides is preferable because it can suppress a decrease in molecular weight and yellowing of the resin during high-temperature melting without impairing high reflectivity.
  • the titanium oxide has at least one inorganic compound selected from the group consisting of a siloxane compound, a silane coupling agent, etc., a group consisting of a polyol, polyethylene glycol, etc., in order to enhance the dispersibility in the resin composition.
  • a siloxane compound e.g., a silane coupling agent, etc.
  • the particle size of the inorganic filler used for the resin layer (A) is arbitrary, and may be appropriately selected and determined according to the use and thickness of the coverlay film of the present invention. In general, a film having a particle size equal to or less than the thickness of the cover lay film is used. Specifically, for example, the average particle size is preferably 0.05 to 50 ⁇ m, more preferably 0.1 to 30 ⁇ m, and particularly preferably about 0. It is preferably 15 to 15 ⁇ m.
  • the particle size of the inorganic filler is 0.05 ⁇ m to 50 ⁇ m because the dispersibility in the resin is good, the interface with the resin is densely formed, and high reflectivity can be imparted.
  • the particle size is preferably 0.1 ⁇ m to 1.0 ⁇ m, and more preferably 0.2 ⁇ m to 0.5 ⁇ m. Is preferred. If the particle size of titanium oxide is in the above range, the dispersibility in the resin is good, the interface with the resin is densely formed, and high reflectivity can be imparted, which is preferable.
  • the content of the inorganic filler used in the resin layer (A) is preferably 10 to 1000 parts by weight, more preferably 20 to 500 parts by weight, and more preferably 25 to 200 parts by weight with respect to 100 parts by weight of the polyorganosiloxane.
  • the amount is preferably 30 to 100 parts by mass. Within this range, it is preferable because good reflection characteristics can be obtained and good reflection characteristics can be obtained even when the film thickness is reduced.
  • the cover lay film includes a resin layer (B) containing a polyorganosiloxane and an inorganic filler different from the inorganic filler contained in the resin layer (A) separately from the resin layer (A). You can also.
  • the resin layer (A) has a high reflectance in the visible light region (400 to 800 nm), and the resin layer (B) has a high reflectance in the ultraviolet (near ultraviolet) region (350 to 400 nm). It is possible to combine resin layers (A) and (B) having different actions such as forming layers.
  • the polyorganosiloxane of the resin layer (B) is not particularly limited as in the case of the resin layer (A) described above, and any conventionally known one may be appropriately selected and determined. Moreover, the means similar to the resin layer (A) mentioned above can also be used for the polyorganosiloxane curing means.
  • the inorganic filler used for the resin layer (B) is not particularly limited as long as it is an inorganic filler different from the inorganic filler contained in the resin layer (A).
  • the inorganic filler used for the resin layer (B) is not particularly limited as long as it is an inorganic filler different from the inorganic filler contained in the resin layer (A).
  • talc mica, mica, glass flake, boron nitride (BN), aluminum nitride, calcium carbonate, aluminum hydroxide, silica, titanate (potassium titanate, etc.), barium sulfate, alumina, kaolin, clay, titanium oxide,
  • Examples thereof include zinc oxide, zinc sulfide, lead titanate, zircon oxide, antimony oxide, and magnesium oxide. These may be added singly or in combination of two or more.
  • the inorganic filler used for the resin layer (A) is titanium oxide, particularly when it is rutile type titanium oxide, light absorption occurs in the ultraviolet (near ultraviolet) region (350 to 400 nm).
  • the inorganic filler used in (B) it is preferable to select anatase-type titanium oxide or alumina that has low light absorption in the 400 nm region.
  • the coverlay film comprising the resin layers (A) and (B) is used for the “substrate for mounting a light-emitting element” described later, anatase-type titanium oxide that absorbs less light in the 400 nm region as an inorganic filler.
  • stack with a metal layer so that the resin layer (B) using an alumina may become a use surface (it may become the exposed side).
  • light in the ultraviolet (near ultraviolet) region 350 to 400 nm
  • light in the visible light region (400 to 800 nm) contains the resin layer (B) and rutile titanium oxide. Therefore, the reflectance can be increased in a wide wavelength region.
  • the particle size of the inorganic filler used for the resin layer (B) is arbitrary, and may be appropriately selected and determined according to the use and thickness of the coverlay film of the present invention. In general, a film having a particle size equal to or less than the thickness of the cover lay film is used.
  • the average particle size is preferably 0.05 to 50 ⁇ m, more preferably 0.1 ⁇ m or more and 30 ⁇ m or less. More preferably, it is 15 ⁇ m or more or 15 ⁇ m or less.
  • the particle size of the inorganic filler is 0.05 ⁇ m to 50 ⁇ m because the dispersibility in the resin is good, the interface with the resin is densely formed, and high reflectivity can be imparted.
  • the content of the inorganic filler used in the resin layer (B) is preferably 10 to 1000 parts by mass with respect to 100 parts by mass of the polyorganosiloxane, more preferably 20 parts by mass or more and 500 parts by mass or less, of which 30 parts by mass. Part or more or 300 parts by mass or less, more preferably 50 parts by mass or more or 200 parts by mass or less. Within this range, it is preferable because good reflection characteristics can be obtained and good reflection characteristics can be obtained even when the film thickness is reduced.
  • the resin layer (A) and the resin layer (B) may contain various additives other than other resins and inorganic fillers as long as the properties are not impaired.
  • a heat stabilizer, an ultraviolet absorber, a light stabilizer, a nucleating agent, a colorant, a lubricant, a flame retardant, and the like may be appropriately blended.
  • the thickness of the cover lay film is not particularly limited and may be appropriately selected and determined. Generally, the thickness is 1 ⁇ m to 1000 ⁇ m, and in the present coverlay film, it is preferably 10 ⁇ m to 1000 ⁇ m. Among them, 10 ⁇ m to 800 ⁇ m, more preferably 20 ⁇ m to 500 ⁇ m, particularly 20 ⁇ m to 300 ⁇ m, and particularly preferably 30 ⁇ m to 200 ⁇ m are preferable. Further, when the effect of the present invention that the rate of decrease in reflectance is small is obtained in a high reflectance region, the thickness of the cover lay film is preferably 50 ⁇ m or more, particularly 100 ⁇ m, The upper limit is usually 1000 ⁇ m, preferably 500 ⁇ m.
  • the thickness is sufficient to seal LED chips and gold wires.
  • the method for preparing the resin composition for forming the resin layer (A) and the resin layer (B), that is, the resin composition for forming the resin layer containing polyorganosiloxane is not particularly limited.
  • a known method can be used.
  • a method of adjusting the concentration of the resin to be mixed and mechanically blending using a kneader or an extruder can be given.
  • (b) a method in which various additives are mechanically blended directly with a resin to be used using a kneader, an extruder, or the like.
  • a method of preparing and mixing the master batch (a) is preferable.
  • a known film forming method for example, an extrusion cast using a T-die using a resin composition obtained by mixing polyorganosiloxane and an inorganic filler.
  • examples thereof include a method of forming a film by a method, a calendering method, or a method of coating on a base film (PET film or the like). What is necessary is just to harden the polyorganosiloxane of an uncrosslinked state by heat curing, radiation curing, etc. for the film formed in this way.
  • This cover lay film can be used as a cover lay film for protecting a conductor circuit of a printed wiring board.
  • a conductor circuit is formed on a substrate, and this cover lay film is laminated on the conductor circuit, while a light emitting element is mounted on the substrate so that the conductor circuit and the light emitting element are electrically connected. can do.
  • the coverlay film it is possible to prevent the conductor circuit from being damaged and disconnected, and to prevent a short circuit due to solder adhesion when the light emitting element is mounted.
  • a light-emitting element mounting substrate (referred to as a “light-emitting element mounting substrate”) according to the second embodiment of the present invention includes a polyorganosiloxane and a substrate used for mounting at least one light-emitting element.
  • a protective layer having a resin layer (A) containing an inorganic filler, the protective layer having an average reflectance of 85% or more at a wavelength of 400 to 800 nm, and a wavelength after heat treatment at 260 ° C. for 10 minutes;
  • the light emitting element mounting substrate is characterized in that a reflectance reduction rate at 450 nm is 5% or less.
  • the light emitting element mounting substrate is not particularly limited in the shape or material of the substrate or the like, and any conventionally known one can be used as long as the above-described conditions are satisfied.
  • a substrate used for mounting a light emitting element is a resin / metal laminate in which a metal layer is laminated on at least one surface of a resin substrate material made of a thermosetting resin or a thermoplastic resin.
  • a configuration in which a wiring pattern (conductor circuit) is formed on at least one surface of the resin substrate material can be exemplified.
  • a protective layer having a resin layer containing a polyorganosiloxane and an inorganic filler having the above-mentioned specific properties is formed on such a “substrate used for mounting a light-emitting element”, that is, the above-mentioned book If a cover lay film is laminated
  • Metal layer examples of the metal layer in the resin / metal laminate used for the light emitting element mounting substrate include copper, gold, silver, aluminum, nickel, tin, and the like.
  • the thickness of the metal layer is arbitrary and may be selected and determined as appropriate, but is usually 1 ⁇ m to 100 ⁇ m, preferably 5 ⁇ m to 70 ⁇ m.
  • copper and copper alloys are preferred as the metal species, and those having the surface subjected to chemical conversion treatment such as black oxidation treatment are preferred.
  • a conductive foil that is a metal layer that has been chemically or mechanically roughened on the contact surface (surface to be overlapped) side with the coverlay film.
  • Specific examples of the conductor foil that has been subjected to the surface roughening treatment include, for example, a roughened copper foil that has been electrochemically treated when an electrolytic copper foil is produced.
  • the resin / metal laminate that is the substrate used for the light emitting element mounting substrate may be a laminate of a plurality.
  • this lamination method a known method can be adopted as a heat fusion method without using an adhesive layer as long as it is a method by heating and pressurization.
  • a heat press method, a heat laminating roll method, and extrusion are used.
  • An extrusion laminating method in which the resin is laminated with a cast roll, or a method combining these can be suitably employed.
  • a metal material such as a copper plate or an aluminum plate, aluminum nitride, or the like is used when more heat dissipation is required. It is also possible to improve heat dissipation by combining with a material having high thermal conductivity such as a ceramic or a graphite plate.
  • the above-mentioned metal laminate is laminated on the entire surface of the aluminum plate, or a window frame for a cavity (recess) structure is removed from the metal laminate and laminated. If you want to.
  • the aluminum to be used is preferably roughened in consideration of the adhesion to the resin, but when considering the cavity structure, in order to efficiently reflect the light from the LED, highly reflective aluminum is used. It is preferable to use it.
  • Examples of the highly reflective aluminum include those whose surfaces have been polished, alumite-treated, and those treated with a reflection-reflecting film in which a metal such as silver is deposited in addition to inorganic oxides such as titanium and silica.
  • the reflectance of aluminum is preferably 80% or more, and more preferably 90% or more, particularly 95% or more, with an average reflectance at a wavelength of 400 to 800 nm.
  • the manufacturing method of this light emitting element mounting substrate is arbitrary, and is not particularly limited.
  • a method for manufacturing a double-sided substrate in which metal layers are laminated on both sides of the substrate will be described with reference to FIG.
  • a substrate (100) made of a thermoplastic resin or a thermosetting resin and two copper foils (10) to be a metal layer are prepared, and (b): A copper foil (10) is laminated on both sides of a substrate (100) made of a thermoplastic resin or a thermosetting resin by a vacuum press to produce a resin / metal laminate.
  • the window cutting method is arbitrary and is not particularly limited. Specifically, for example, a method using a big die, a router processing method, a laser processing method, or the like can be used.
  • the protective layer may be formed by applying a resin layer (30) containing polyorganosiloxane and an inorganic filler.
  • a manufacturing method of the light emitting element mounting substrate as the aluminum composite substrate will be described with reference to FIG.
  • FIG. 2 (a): a copper foil (10) is laminated on one side of a substrate (100) made of a thermoplastic resin or a thermosetting resin to produce a metal laminate. And (b): The copper foil (10) is etched to form a wiring pattern (20), gold plating is performed, and the substrate (100) is punched into a cavity frame using a big die (50).
  • the method of punching into the cavity frame is not limited to the above method using the Bic die, and can be formed by, for example, router processing or laser.
  • stacking of the film with a single-sided copper foil ((b) in FIG. 2), a protective layer, and an aluminum plate is performed collectively, these are laminated
  • a conductor pattern may be formed.
  • a conductive circuit is formed on the substrate for mounting the light emitting element, and the substrate and the light emission mounted on the substrate.
  • the element is electrically connected and the light emitting element is sealed with resin.
  • a conductor circuit is formed on a substrate, a protective layer is laminated on the conductor circuit, and the light emitting element on the substrate is mounted to make the conductor circuit and the light emitting element conductive, and the light emitting element.
  • the protective layer in the light source device has the characteristics of the resin layer (A), for example, the average reflectance at a wavelength of 400 to 800 nm is 85% or more, and the wavelength is 450 nm after heat treatment at 260 ° C. for 10 minutes. In other words, the reflectance is decreased by 5% or less. Therefore, by forming the protective layer in this way, it becomes possible to effectively protect the conductor circuit, which causes a decrease in reflectivity even under high temperature heat load environment and light resistance test environment. Therefore, the light source device of the present invention can be used for various applications such as lighting, projector light sources, backlight devices such as liquid crystal display devices, in-vehicle applications, and mobile phone applications.
  • Sheet generally refers to a product that is thin by definition in JIS and generally has a thickness that is small and flat for the length and width.
  • film is compared to the length and width.
  • a film having a thickness of 100 ⁇ m or more is sometimes referred to as a sheet, and a film having a thickness of less than 100 ⁇ m is sometimes referred to as a film.
  • X is preferably greater than X” or “preferably Y”, with the meaning of “X to Y” unless otherwise specified. It also includes the meaning of “smaller”.
  • X or more is an arbitrary number
  • Y or less is an arbitrary number
  • An integrating sphere is attached to a spectrophotometer ("U-4000", manufactured by Hitachi, Ltd.), and the reflectance when the reflectance of the alumina white plate is assumed to be 100% is measured at intervals of 0.5 nm over a wavelength range of 400 nm to 800 nm. It was measured. The average value of the measured values obtained was calculated, and this value was taken as the average reflectance. The average reflectance at a wavelength of 350 to 400 nm was measured in the same manner.
  • the obtained white film was fixed with a fixing jig, heated in a hot air circulation oven at 260 ° C. for 10 minutes, the reflectance after the heat treatment was measured in the same manner as described above, and the reflectance at 450 nm was read. It was.
  • the obtained coverlay film was temperature 63 ° C. (black panel temperature), humidity 50%, irradiance (295 to 400 nm) 60 W / m. 2 was irradiated for 50 hours, followed by measuring the above method as well as the reflectance was read reflectance at 450nm.
  • Example 1 Resin obtained by mixing 100 parts by mass of polyorganosiloxane (TSE2571-5U, manufactured by Momentive) and 67 parts by mass of rutile type titanium oxide (R105, manufactured by DuPont, average particle size 0.31 ⁇ m) with a planetary mixer.
  • a coverlay film precursor having a thickness of 100 ⁇ m was obtained on the release PET film at a set temperature of 100 ° C. using an extruder.
  • cure by the irradiation dose of 50 kGy with a gamma ray was evaluated by the method mentioned above. The results are shown in Table 1.
  • Example 2 1.5 parts by mass of a vulcanizing agent (TC-12, manufactured by Momentive) as a thermal crosslinking material and 100 parts by mass of polyorganosiloxane (TSE2571-5U, manufactured by Momentive), titanium oxide (R105, manufactured by DuPont) , Average particle size 0.31 ⁇ m)
  • TC-12 vulcanizing agent
  • TSE2571-5U polyorganosiloxane
  • R105 titanium oxide
  • Example 3 A coverlay film made of the resin layer (A) was prepared and evaluated in the same manner as in Example 1 except that the thickness was 300 ⁇ m. The results are shown in Table 1.
  • Example 4 A coverlay film made of the resin layer (A) was produced and evaluated in the same manner as in Example 1 except that the titanium oxide was changed to 400 parts by mass. The results are shown in Table 1.
  • Example 5 A coverlay film made of the resin layer (A) was prepared and evaluated in the same manner as in Example 1 except that the titanium oxide was changed to 25 parts by mass. The results are shown in Table 1.
  • Example 6 A coverlay film made of the resin layer (A) was produced and evaluated in the same manner as in Example 1 except that the thickness was 50 ⁇ m. The results are shown in Table 1.
  • Example 7 The resin layer (A) was prepared in the same manner as in Example 1 except that 25 parts by mass of anatase-type titanium oxide (SA-1, Sakai Chemical Industry Co., Ltd., average particle size: 0.3 ⁇ m) was used as titanium oxide. A coverlay film consisting of was prepared and evaluated. The results are shown in Table 1.
  • SA-1 Sakai Chemical Industry Co., Ltd., average particle size: 0.3 ⁇ m
  • Example 8 A coverlay film composed of the resin layer (A) was prepared and evaluated in the same manner as in Example 1 except that polyorganosiloxane (TSE2913-U, manufactured by Momentive) was used as the polyorganosiloxane. The results are shown in Table 1.
  • Example 9 A cover lay film comprising a resin layer (A) in the same manner as in Example 1 except that 150 parts by mass of alumina (AA04, manufactured by Sumitomo Chemical Co., Ltd., average particle size 0.4 ⁇ m) was used instead of titanium oxide. Were made and evaluated. The results are shown in Table 1.
  • Example 10 A coverlay film made of the resin layer (A) was prepared and evaluated in the same manner as in Example 8 except that the thickness was 150 ⁇ m. The results are shown in Table 1.
  • Example 11 A coverlay film made of the resin layer (A) was prepared and evaluated in the same manner as in Example 9 except that the thickness was 150 ⁇ m. The results are shown in Table 1.
  • Example 12 After obtaining a coverlay film precursor composed of a resin layer (A) having a thickness of 100 ⁇ m by the same method as in Example 8, the resin layer (B) having a thickness of 50 ⁇ m was obtained in the same manner as in Example 9. A coverlay film precursor was prepared, and the coverlay film surfaces of both precursors were bonded together, and then a coverlay film having a laminated structure cured with ⁇ rays was prepared and evaluated. The results are shown in Table 1. In addition, the measurement of the reflectance measured the surface which consists of a resin layer (B).
  • Example 13 A coverlay film having a laminated structure was prepared and evaluated in the same manner as in Example 12 except that the thickness of the resin layer (B) was 100 ⁇ m. The results are shown in Table 1. In addition, the measurement of the reflectance measured the surface which consists of a resin layer (B).
  • Example 1 to 8 and 10 since polyorganosiloxane was filled with titanium oxide, the reflectance was particularly high even in the visible light region (400 to 800 nm). Since Example 7 was filled with anatase-type titanium oxide, the reflectivity in the ultraviolet region was higher than that of Examples 1 to 6, 8, and 10 filled with rutile type.
  • Example 12 and 13 by setting it as the laminated structure of the resin layer (A) which filled the polyorganosiloxane with the rutile type titanium oxide, and the resin layer (B) which filled the polyorganosiloxane with the alumina, High reflectivity was exhibited in both the ultraviolet light region (350 to 400 nm) and the visible light region (400 to 800 nm).

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Abstract

Cette invention concerne une couche de fermeture particulièrement destinée à une carte de circuit imprimé sur laquelle doit être montée une DEL, et un dispositif formant source d'éclairage. Ladite couche de fermeture présente une réflectivité élevée dans une plage de lumière visible, une faible dégradation de la réflectivité même dans un environnement à charge thermique élevée et dans un environnement d'essai de la résistance à la lumière, et elle peut accueillir des cartes de circuit imprimé de grande superficie. Ladite couche de fermeture est conçue pour protéger un circuit conducteur d'une carte de circuit imprimé et elle est dotée d'une couche de résine qui contient un polyorganosiloxane et une charge inorganique. La réflectivité moyenne de la couche de fermeture dans une plage de longueurs d'onde allant de 400 à 800 nm est supérieure ou égale à 85 % et leur baisse de réflectivité à une longueur d'onde de 450 nm est inférieure ou égale à 5 % telle qu'elle a été déterminée après traitement thermique à 260 °C pendant 10 minutes.
PCT/JP2013/052685 2012-02-10 2013-02-06 Couche de fermeture, carte de circuit imprimé à équiper d'un élément électroluminescent et dispositif formant source d'éclairage WO2013118752A1 (fr)

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JP2013557536A JP5676785B2 (ja) 2012-02-10 2013-02-06 カバーレイフィルム、発光素子搭載用基板、及び光源装置
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JP2018060989A (ja) * 2016-10-04 2018-04-12 日本特殊陶業株式会社 枠体部材、発光装置、およびこれらの製造方法
JP2018085368A (ja) * 2016-11-21 2018-05-31 日本特殊陶業株式会社 蓋部材、該蓋部材を用いた発光装置、およびこれらの製造方法
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JP2016103576A (ja) * 2014-11-28 2016-06-02 三菱樹脂株式会社 蛍光体含有シリコーンシート及び発光装置
JP2018060989A (ja) * 2016-10-04 2018-04-12 日本特殊陶業株式会社 枠体部材、発光装置、およびこれらの製造方法
JP2018085368A (ja) * 2016-11-21 2018-05-31 日本特殊陶業株式会社 蓋部材、該蓋部材を用いた発光装置、およびこれらの製造方法
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