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WO2016017818A1 - Réflecteur et composition de résine - Google Patents

Réflecteur et composition de résine Download PDF

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Publication number
WO2016017818A1
WO2016017818A1 PCT/JP2015/071880 JP2015071880W WO2016017818A1 WO 2016017818 A1 WO2016017818 A1 WO 2016017818A1 JP 2015071880 W JP2015071880 W JP 2015071880W WO 2016017818 A1 WO2016017818 A1 WO 2016017818A1
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WO
WIPO (PCT)
Prior art keywords
reflector
mass
resin composition
resin
white pigment
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/JP2015/071880
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English (en)
Japanese (ja)
Inventor
智紀 佐相
勝哉 坂寄
恵維 天下井
了 管家
俊之 坂井
慶介 橋本
弘侑 長谷川
誠 溝尻
前田　晃宏
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Dai Nippon Printing Co Ltd
Original Assignee
Dai Nippon Printing Co Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Priority claimed from JP2014157978A external-priority patent/JP2016035010A/ja
Application filed by Dai Nippon Printing Co Ltd filed Critical Dai Nippon Printing Co Ltd
Publication of WO2016017818A1 publication Critical patent/WO2016017818A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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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
    • C08J7/00—Chemical treatment or coating of shaped articles made of macromolecular substances
    • 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
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
    • C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
    • C08L23/18—Homopolymers or copolymers of hydrocarbons having four or more carbon atoms
    • C08L23/20—Homopolymers or copolymers of hydrocarbons having four or more carbon atoms having four to nine carbon atoms
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10H—INORGANIC LIGHT-EMITTING SEMICONDUCTOR DEVICES HAVING POTENTIAL BARRIERS
    • H10H20/00—Individual inorganic light-emitting semiconductor devices having potential barriers, e.g. light-emitting diodes [LED]
    • H10H20/80—Constructional details
    • H10H20/85—Packages
    • H10H20/855—Optical field-shaping means, e.g. lenses
    • H10H20/856—Reflecting means
    • 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
    • H01L2224/01—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
    • H01L2224/481—Disposition
    • H01L2224/48151—Connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive
    • H01L2224/48221—Connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive the body and the item being stacked
    • H01L2224/48245—Connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive the body and the item being stacked the item being metallic
    • H01L2224/48247—Connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive the body and the item being stacked the item being metallic connecting the wire to a bond pad of the item
    • 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
    • H01L2224/484—Connecting portions
    • H01L2224/4847—Connecting portions the connecting portion on the bonding area of the semiconductor or solid-state body being a wedge bond
    • H01L2224/48472—Connecting portions the connecting portion on the bonding area of the semiconductor or solid-state body being a wedge bond the other connecting portion not on the bonding area also being a wedge bond, i.e. wedge-to-wedge
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2924/00—Indexing scheme for arrangements or methods for connecting or disconnecting semiconductor or solid-state bodies as covered by H01L24/00
    • H01L2924/15—Details of package parts other than the semiconductor or other solid state devices to be connected
    • H01L2924/181—Encapsulation
    • H01L2924/183—Connection portion, e.g. seal
    • H01L2924/18301—Connection portion, e.g. seal being an anchoring portion, i.e. mechanical interlocking between the encapsulation resin and another package part

Definitions

  • the present invention relates to a reflector and a resin composition.
  • the substrate is heated by means of infrared rays, hot air, etc.
  • a method (reflow method) for melting and fixing electronic components is employed. By this method, the mounting density of electronic components on the substrate surface can be improved.
  • an LED element which is one of semiconductor light emitting devices, is widely used as a light source such as an indicator lamp because of its small size, long life, and excellent power saving.
  • LED elements with higher brightness have been manufactured at a relatively low cost, and therefore, use as a light source to replace fluorescent lamps and incandescent bulbs has been studied.
  • a plurality of LED elements are arranged on a surface-mounted LED package, that is, a metal substrate (LED mounting substrate) such as aluminum, and each LED element.
  • a system is often used in which a reflector (reflector) that reflects light in a predetermined direction is disposed around the.
  • the LED element since the LED element generates heat during light emission, in such a type of LED lighting device, the reflector deteriorates due to the temperature rise during light emission of the LED element, and the reflectance decreases, thereby reducing the brightness. The life of the element will be shortened. Therefore, heat resistance is required for the reflector.
  • Patent Document 1 proposes a polymer composition used for a reflector of a light emitting diode, specifically, polyphthalamide, carbon black, titanium dioxide, glass fiber, and an antioxidant.
  • a polymer composition is disclosed.
  • the reflectance after heat aging is measured about the said composition, Compared with the polymer composition which does not contain carbon black, the favorable reflectance is obtained with the said composition, and it has shown that there is also little yellowing.
  • the heat aging test of the polymer composition described in Patent Document 1 is an evaluation in a short time of 3 hours at 170 ° C., and good results can be obtained with heat resistance and durability under a longer practical condition. Whether it is unknown.
  • Patent Document 2 discloses a thermosetting light reflecting resin composition used for an optical semiconductor device in which an optical semiconductor element and a wavelength conversion means such as a phosphor are combined.
  • the heat aging test of the thermosetting light reflecting resin composition described in Patent Document 2 has been verified under a more practical condition of 150 hours at 150 ° C., but the molding time is 90 seconds compared to the thermoplastic resin. Since it is long and requires 2 hours as post-cure at 150 ° C., there is a problem in productivity.
  • Patent Document 3 discloses an olefin resin, a crosslinking agent having an allylic substituent having a molecular weight of 1000 or less, inorganic particles such as spherical fused silica and glass fiber, and a white pigment.
  • the resin composition containing these is described.
  • a resin composition has the outstanding heat resistance, it is described that it is useful when producing molded objects, such as a reflector, through a reflow process.
  • Patent Document 3 proposes an electron beam curable resin composition containing polymethylpentene and a crosslinking agent having an allylic substituent having a molecular weight of 1000 or less.
  • the electron beam curable composition containing a white pigment and further containing inorganic particles other than the white pigment has excellent heat resistance in the reflow process, and formed into a molded body such as a reflector. It is described that excellent heat resistance can be obtained.
  • a white pigment and inorganic particles sinherical fused silica, glass fiber
  • 105 parts by mass is the maximum with respect to 100 parts by mass of pentene, and there is no description about including more white pigments and inorganic particles.
  • an object of the first invention is to provide a reflector having excellent adhesion to a substrate while maintaining at least basic performances such as required heat resistance and reflectance.
  • the gist of the first invention is as follows.
  • the present inventors solved the said subject by using the fibrous filler which has a specific cross-sectional area in radial direction. That is, a reflector having a light reflection surface formed from a resin composition containing a resin and an inorganic filler containing a white pigment and a fibrous filler, and the radial cross-sectional area of the fibrous filler is 1 ⁇ m 2. 100 ⁇ m 2 or less, and using a thermogravimetric / differential thermal simultaneous analyzer based on the TG-DTA method, after measuring the mass of the reflector before heating, up to 600 ° C. at 10 ° C./min in an air atmosphere A reflector in which the amount of ash remaining after heating at 600 ° C. for 30 minutes after heating is 70% or more and 90% or less based on the total mass of the reflector before heating.
  • the gist of the second invention is as follows.
  • a resin composition comprising more than 500 parts by mass and less than 500 parts by mass.
  • the first invention it is possible to provide a reflector having excellent adhesion to a substrate while maintaining at least basic performances such as required heat resistance and reflectance.
  • the second invention it is possible to provide a resin composition capable of obtaining a molded body having no white color tone and excellent in heat resistance without cracks when formed into a molded body.
  • first embodiment an embodiment according to the first invention
  • second embodiment an embodiment according to a second invention
  • the first invention and the second invention are not limited to the embodiments described below.
  • the reflector according to the first embodiment of the present invention is molded from a resin composition containing a resin and an inorganic filler including a white pigment and a fibrous filler (hereinafter, sometimes referred to as a resin composition for reflector).
  • the radial filler has a radial cross-sectional area of 1 ⁇ m 2 or more and 100 ⁇ m 2 or less using a thermogravimetric / differential thermal analyzer based on the TG-DTA method. After measuring the mass of the reflector before heating, the amount of ash remaining after heating at 600 ° C. for 30 minutes after heating up to 600 ° C. in an air atmosphere is based on the total mass of the reflector before heating.
  • the ash content of the reflector according to this embodiment is less than 70% by mass, the heat resistance required in the reflow process cannot be satisfied. Moreover, when the amount of ash exceeds 90 mass%, the moldability of a reflector will fall. From the above viewpoint, the lower limit of the ash content is preferably 72% by mass, and more preferably 75% by mass. Moreover, it is preferable that the upper limit of the said ash content is 88 mass%, and it is more preferable that it is 85 mass%.
  • the reflector according to the embodiment of the present invention mainly has an action of reflecting light from the LED element of the semiconductor light emitting device toward the lens (light emitting portion).
  • the reflector according to the present embodiment may be used in combination with a semiconductor light emitting device described later, or may be used in combination with a semiconductor light emitting device made of another material, an LED mounting substrate, or the like. Details of the reflector are the same as those of the reflector (reflector 12 in FIGS. 1 and 2) applied to the semiconductor light emitting device described later with reference to FIGS.
  • the reflector according to the present embodiment can be applied to various uses. For example, the present invention can be applied to a heat-resistant insulating film, a heat-resistant release sheet, a light reflecting sheet of a solar cell, lighting such as an LED, a reflector for a light source for a television, and the like.
  • the sealing property of the optical semiconductor element affects the life of the semiconductor element.
  • the reflector according to the present embodiment has good adhesion and high sealing performance. It can be preferably applied to.
  • the present invention can be more suitably applied to a metal substrate type LED that is formed by processing a lead frame by etching and half etching and uses the back surface of the element installation portion as an electrode.
  • the resin composition for reflectors that can be used for molding the light reflecting surface of the reflector according to the first embodiment of the present invention contains at least a resin and an inorganic filler containing a white pigment and a fibrous filler.
  • the resin that can be used in the first embodiment may be any resin that can be used for molding the light reflecting surface, and examples thereof include polyamide, polycarbonate, acrylic resin, polyacetal, polyethylene terephthalate, and polystyrene. Among these, it is preferable to use a polyolefin resin.
  • the resins may be used alone, or different resins can be blended and used. Furthermore, block polymers, copolymers and terpolymers obtained from different monomers may be used.
  • the polyolefin resin include resins obtained by ring-opening metathesis polymerization of polyethylene, polypropylene, polybutene, polymethylpentene, and norbornene derivatives, or hydrogenated resins thereof.
  • the polyolefin resin at least one selected from polyethylene, polypropylene, polyethylene containing a cyclic structure, polypropylene containing a cyclic structure, and polymethylpentene is preferable.
  • Polymethylpentene has a high melting point of 230 to 240 ° C., does not decompose even at a molding temperature of about 280 ° C., and has excellent chemical resistance and electrical insulation properties.
  • a polyolefin resin such as polymethylpentene can be suitably used for a reflector of a semiconductor light emitting device, for example.
  • the polymethylpentene resin is preferably a homopolymer of 4-methylpentene-1, but 4-methylpentene-1 and other ⁇ -olefins such as ethylene, propylene, 1-butene, 1-pentene, 1-pentene, ⁇ having 2 to 20 carbon atoms such as hexene, 1-octene, 1-decene, 1-dodecene, 1-tetradecene, 1-octadecene, 1-eicocene, 3-methyl-1-butene, 3-methyl-1-pentene, etc.
  • -Copolymers with olefins mainly 4-methyl-1-pentene.
  • the polyolefin resin that can be used in the reflector resin composition preferably has a weight average molecular weight of 220,000 to 800,000.
  • the weight average molecular weight of the polyolefin resin is in the above range, the occurrence of cracks in a molded article such as a reflector obtained by molding a resin composition for a reflector containing the polyolefin resin can be suppressed. For example, the destruction of the reflector in the reflow process Etc. can be prevented.
  • the lower limit of the weight average molecular weight is preferably 230,000 or more, more preferably 240,000 or more.
  • the upper limit of the weight average molecular weight is preferably 700,000 or less, more preferably 650,000 or less.
  • the weight average molecular weight is preferably a polystyrene equivalent weight average molecular weight measured by gel permeation chromatography (GPC).
  • GPC gel permeation chromatography
  • the method is not limited to this as long as the method can measure the weight average molecular weight with good reproducibility.
  • the weight average molecular weight can be measured by a method exemplified for a material extracted with an appropriate solvent.
  • An example of conditions for measuring the weight average molecular weight by GPC is as follows. Eluent: o-dichlorobenzene Temperature: 140-160 ° C Flow rate: 1.0 mL / min Sample concentration: 1.0 g / L Injection volume: 300 ⁇ L
  • the inorganic filler which can be used for the resin composition for reflectors contains a white pigment and a fibrous filler.
  • the inorganic filler will be described.
  • white pigment titanium oxide, zinc sulfide, zinc oxide, barium sulfide, potassium titanate and the like can be used alone or in combination as white pigments that can be used in the resin composition for reflectors.
  • the white pigment is used for imparting a white color tone to the molded product obtained from the resin composition, and particularly improves the light reflectance of the molded product by setting the color tone to a high white color. be able to.
  • the average particle diameter of the white pigment is preferably 0.10 ⁇ m or more and 0.50 ⁇ m or less, and 0.10 ⁇ m or more and 0.40 ⁇ m or less in the primary particle size distribution from the viewpoint of obtaining moldability and obtaining high reflectance. It is more preferable that it is 0.21 ⁇ m or more and 0.25 ⁇ m or less.
  • An average particle diameter can be calculated
  • the inorganic filler usable in the reflector for the resin composition required to include fibrous fillers requires that the cross-sectional area in the radial direction of the fibrous filler is 1 [mu] m 2 or more 100 [mu] m 2 or less .
  • the cross-sectional area in the radial direction of the fibrous filler is less than 1 ⁇ m 2 , the filler strength is reduced and the fiber is easily broken or broken in the fiber length direction during processing. As a result, the length is shortened. Sexuality decreases.
  • the cross-sectional area of the fibrous filler in the present embodiment is an actual measurement obtained by breaking the reflector of the semiconductor light-emitting device and observing the broken cross-section with an SEM. It shall be calculated from the value. That is, in the SEM image, the diameter length of the fibrous filler appearing in the cross section of the reflector is measured.
  • the cross section of the filler has an elliptical shape
  • the major axis and minor axis of the ellipse are measured, and the ratio of the major axis to the minor axis is 0.8 to 1.2, and at least 10
  • the average value about a cross section be a cross-sectional area of a fibrous filler.
  • the diameter is measured up to three significant digits.
  • the cross-sectional area is calculated as the average value of the cross-sectional area of the fibrous filler from the smallest cross-sectional area to the 50% of the total number of measurements, and the calculated value is rounded off to the third digit. To do.
  • the lower limit value of the cross-sectional area in the radial direction of the fibrous filler is preferably 30 ⁇ m 2 , and more preferably 35 ⁇ m 2 .
  • the upper limit of the cross-sectional area in the radial direction of the fibrous filler is preferably a 85 .mu.m 2, more preferably 50 [mu] m 2.
  • fibrous fillers include asbestos fibers, carbon fibers, graphite fibers, metal fibers, slag fibers, gypsum fibers, silica fibers, silica-alumina fibers, zirconia fibers, boron nitride fibers, silicon nitride fibers, boron fibers, glass fibers, etc. Can be mentioned.
  • the fibrous filler is a glass fiber containing 60% by mass or more of silicon dioxide from the viewpoint of forming the light reflecting surface of the reflector and improving the light reflectance.
  • the ratio of silicon dioxide in the fibrous filler is more preferably 65% by mass or more, and further preferably 70% by mass or more.
  • the cross-sectional shape of the fibrous filler may be a general, substantially circular shape, or an irregular cross-section such as a flat shape.
  • the fiber does not have to have a constant cross-sectional shape and cross-sectional area.
  • the cross-sectional performance in this case is defined as a cross-sectional area obtained by averaging different cross-sectional areas in the length direction.
  • the size of the cross section satisfies the above-mentioned definition of the cross sectional area
  • the short axis D1 of the cross section is 0.5 ⁇ m or more and 25 ⁇ m or less
  • the long diameter D2 is 0.5 ⁇ m.
  • the ratio D2 / D1 of D2 to D1 is 1.0 to 30 and 300 ⁇ m or less.
  • the average fiber length of glass fiber is 0.75 micrometer or more and 300 micrometers or less.
  • Such glass fibers are also called milled fibers, and can be obtained by pulverizing long fibers.
  • the reflector resin composition in addition to the white pigment and the fibrous filler, is usually a thermoplastic resin composition; a thermosetting resin composition such as an epoxy resin, an acrylic resin, or a silicone resin, and an inorganic filler. As long as it does not interfere with the reflection characteristics as a reflector, can be used alone or in combination.
  • Examples include aluminum borate whiskers, magnesium whiskers, silicon whiskers, wollastonite, imogolite, sepiolite, zonolite, silica particles, layered silicates, layered silicates exchanged with organic onium ions, glass flakes, non-swelling Carbon nanoparticles such as synthetic mica, graphite, metal foil, ceramic beads, clay, mica, sericite, zeolite, bentonite, dolomite, kaolin, powdered silicic acid, feldspar powder, shirasu balloon, gypsum, novaculite, dosonite, and white clay fullerene Examples thereof include plate-like and particulate inorganic fillers.
  • the resin composition for reflectors may contain the crosslinking agent further.
  • the resin composition contains a crosslinking agent, it is shaped into a reflector shape, and then irradiated with an electron beam to obtain a reflector. Thereby, the more outstanding heat resistance can be provided to the reflector which concerns on this embodiment.
  • the crosslinking agent has at least one ring structure that is saturated or unsaturated, and at least one atom forming the ring structure includes an allyl group, a methallyl group, an allyl group via a linking group, and a linking group. It has a structure in which any allylic substituent of the methallyl group via is bonded.
  • the resin composition in the first embodiment exhibits good electron beam curability and has excellent heat resistance by containing a crosslinking agent having such a structure.
  • the saturated or unsaturated ring structure include a cyclo ring, a hetero ring, and an aromatic ring.
  • the number of atoms forming the ring structure is preferably 3 to 12, more preferably 5 to 8, and still more preferably a 6-membered ring.
  • the number of ring structures is preferably 1 to 3, more preferably 1 or 2, and still more preferably 1.
  • the molecular weight of the crosslinking agent is preferably 1000 or less, more preferably 500 or less, and even more preferably 300 or less. When the molecular weight is 1000 or less, good dispersibility is obtained in the resin composition, and it is possible to cause an effective crosslinking reaction by electron beam irradiation.
  • the melting point of the crosslinking agent is preferably not higher than the melting point of the polyolefin resin to be used, and is preferably 200 ° C. or lower, for example.
  • the molding temperature of the resin composition is reduced to reduce the thermal load, friction during molding, and the inorganic filler containing a white pigment.
  • the content rate can be increased.
  • linking group in the crosslinking agent examples include an ester bond, an ether bond, an alkylene group, and a (hetero) arylene group.
  • atoms forming the ring atoms that are not bonded to the allylic substituent are in a state in which hydrogen, oxygen, nitrogen, or the like is bonded, or in a state in which various substituents are bonded.
  • an allylic substituent is independently bonded to at least two atoms forming one ring of the crosslinking agent. It is preferable that When the ring structure is a 6-membered ring, it is preferable that an allylic substituent is preferably bonded to at least two of the atoms forming the ring independently of each other. It is preferable that another allylic substituent is bonded to the meta position of the bonded atom.
  • the crosslinking agent is preferably represented by the following formula (1) or (2).
  • R 1 to R 3 are each independently an allylic substituent of any one of an allyl group, a methallyl group, an allyl group via an ester bond, and a methallyl group via an ester bond.
  • R 1 to R 3 are each independently an allylic substituent of any one of an allyl group, a methallyl group, an allyl group via an ester bond, and a methallyl group via an ester bond.
  • crosslinking agent represented by the above formula (1) examples include triallyl isocyanurate, methyl diallyl isocyanurate, diallyl monoglycidyl isocyanuric acid, monoallyl diglycidyl isocyanurate, and trimethallyl isocyanurate.
  • crosslinking agent represented by the above formula (2) examples include orthophthalic acid diallyl ester, isophthalic acid diallyl ester, and the like.
  • an elastomer may be blended with the polyolefin resin as necessary for the purpose of improving moldability and physical properties as a reflector.
  • the elastomer is a polymer having a glass transition temperature of 40 ° C. or less, and includes a normal rubbery polymer and a thermoplastic elastomer.
  • the glass transition temperature is two or more in the case of a block copolymerized rubber polymer or the like
  • the rubbery polymer having a glass transition temperature of 40 ° C. or less according to the present invention if the lowest glass transition temperature is 40 ° C. or less. Can be used as
  • elastomers include isoprene rubber, hydrogenated product thereof; chloroprene rubber, hydrogenated product thereof; saturated polyolefin such as ethylene / propylene copolymer, ethylene / ⁇ -olefin copolymer, propylene / ⁇ -olefin copolymer Rubber: Ethylene / propylene / diene copolymer, ⁇ -olefin / diene copolymer, isobutylene / isoprene copolymer, diene copolymer such as isobutylene / diene copolymer, their halides, diene polymer Or hydrogenated products thereof; acrylonitrile / butadiene copolymer, hydrogenated products thereof; vinylidene fluoride / trifluoride ethylene copolymer, vinylidene fluoride / hexafluoropropylene copolymer, vinylidene fluoride / six Prop
  • Thermoplastic elastomers such as thermoplastic elastomers, 1,2-polybutadiene-based thermoplastic elastomers, vinyl chloride-based thermoplastic elastomers, fluorine-based thermoplastic elastomers; A melted one is mentioned.
  • a copolymer of an aromatic vinyl monomer and a conjugated diene monomer, and a hydrogenated product thereof are preferable because of good dispersibility with the alicyclic structure-containing thermoplastic resin.
  • the copolymer of the aromatic vinyl monomer and the conjugated diene monomer may be a block copolymer or a random copolymer. From the viewpoint of weather resistance, hydrogenated portions other than aromatic rings are more preferable.
  • styrene / butadiene block copolymer styrene / butadiene / styrene / block copolymer, styrene / isoprene / block copolymer, styrene / isoprene / styrene / block copolymer, and hydrogenated products thereof.
  • the reflector resin composition may contain various additives as long as the function of the reflector formed from the reflector resin composition is not impaired.
  • Additives can be blended.
  • a dispersant such as a silane coupling agent can be blended in the reflector resin composition.
  • the silane coupling agent include disilazane such as hexamethyldisilazane; cyclic silazane; trimethylsilane, trimethylchlorosilane, dimethyldichlorosilane, methyltrichlorosilane, allyldimethylchlorosilane, trimethoxysilane, benzyldimethylchlorosilane, Methyltrimethoxysilane, methyltriethoxysilane, isobutyltrimethoxysilane, dimethyldimethoxysilane, dimethyldiethoxysilane, trimethylmethoxysilane, hydroxypropyltrimethoxysilane, phenyltrimethoxysilane, n-butyltrimethoxysilane, n-hexadecyl Trime
  • the reflector resin composition may be formed into a granulated product such as a pellet by melt-kneading the polyolefin resin described above and an inorganic filler containing a white pigment and a fibrous filler.
  • a melt-kneading method such as a melt-kneading extruder, a two-roll or three-roll, a stirrer such as a homogenizer or a planetary mixer, or a melt-kneader such as a polylab system or a lab plast mill is used. be able to.
  • the resin content is preferably 7% by mass or more and 30% by mass or less based on the total mass of the reflector resin composition.
  • the lower limit value of the resin content is more preferably 10% by mass, and even more preferably 11% by mass.
  • the upper limit value of the resin content is more preferably 28% by mass, and further preferably 25% by mass or less. If the content rate of resin is the said range, it can be set as the molded object excellent in heat resistance, maintaining the moldability at the time of shape
  • 70 mass% or more is preferable on the basis of the total mass of the resin composition for reflectors, and, as for the inorganic filler content rate in the resin composition for reflectors, More preferably, it is 72 mass% or more, More preferably Is 75% by mass or more.
  • the upper limit of the inorganic filler content is about 90% by mass from the viewpoint of moldability.
  • content of a white pigment shall be more than 200 mass parts and 500 mass parts or less with respect to 100 mass parts of resin from viewpoints of product performance, such as the light reflectance of a reflector, intensity
  • the content of the white pigment is more than 200 parts by mass with respect to 100 parts by mass of the resin, sufficient product performance can be obtained in terms of the light reflectivity, strength, molding warp, etc. of the reflector.
  • the content of the white pigment in the inorganic filler is preferably 10 parts by mass or more and 300 parts by mass or less, more preferably 30 parts by mass or more and 200 parts by mass or less, and 50 parts by mass with respect to 100 parts by mass of the resin. More preferably, it is 180 parts by mass or less.
  • content of the fiber filler in an inorganic filler By making content of the fiber filler in an inorganic filler into the said range, the heat resistance requested
  • content of a crosslinking agent when a crosslinking agent is contained in the resin composition for reflectors, content of a crosslinking agent is 15 mass parts or more and 40 mass parts or less with respect to 100 mass parts of resin, Preferably it is 15 The amount can be not less than 30 parts by mass and more preferably not less than 16 parts by mass and not more than 20 parts by mass. If the crosslinking agent is within the above range, crosslinking can be carried out effectively without bleeding out the crosslinking agent from the molded product before crosslinking.
  • the amount of ash based on the TG-DTA method of the resin composition for reflectors needs to be 70% by mass or more and 90% by mass or less based on the total mass of the resin composition for reflectors before heating.
  • the amount of ash based on the TG-DTA method is the same as the above-mentioned conditions, and after measuring the mass before heating of the resin composition for reflector using a thermogravimetric / differential thermal analyzer, This is the amount of ash remaining after heating to 600 ° C. at 10 ° C./min and heating at 600 ° C. for 30 minutes.
  • the ash content of the resin composition for a reflector is less than 70% by mass, the heat resistance required in the reflow process and the required reflectance cannot be satisfied. Moreover, when the amount of ash exceeds 90 mass%, the moldability of a reflector will fall. From the above viewpoint, the lower limit of the ash content is preferably 72% by mass, and more preferably 75% by mass. Moreover, it is preferable that the upper limit of the said ash content is 88 mass%, and it is more preferable that it is 85 mass%.
  • molding methods such as transfer molding, compression molding, and injection molding
  • molding methods can be used.
  • a molded article having a reflector shape can be obtained by injection molding at a cylinder temperature of 200 to 400 ° C. and a mold temperature of 20 to 150 ° C.
  • a crosslinking agent is used, a more cured reflector can be obtained by subjecting the obtained molded body to electron beam irradiation treatment.
  • the heat resistance of the reflector can be further enhanced by performing the electron beam irradiation treatment.
  • the electron beam irradiation treatment may be performed on the resin composition for reflectors before molding, or the resin composition for reflectors after the electron beam irradiation treatment may be molded into a desired shape as a reflector.
  • the acceleration voltage of an electron beam it can select suitably according to the magnitude
  • the used crosslinking agent can be crosslinked and cured usually at an acceleration voltage of about 250 to 3000 kV.
  • the transmission capability increases as the acceleration voltage increases. Therefore, when using a base material that deteriorates due to the electron beam as the base material, the transmission depth of the electron beam and the thickness of the molded body are substantially equal.
  • the accelerating voltage so as to be equal to each other, it is possible to suppress irradiation of an excessive electron beam to the molded body, and to minimize degradation of the molded body due to excess electron beams.
  • the absorbed dose when irradiating with an electron beam is appropriately set depending on the composition of the resin composition, but the amount at which the crosslink density in the molded body is saturated is preferable, and the irradiated dose is preferably 50 to 600 kGy.
  • the electron beam source is not particularly limited.
  • various electron beam accelerators such as a cockroft Walton type, a bandegraft type, a resonant transformer type, an insulated core transformer type, a linear type, a dynamitron type, a high frequency type, etc. Can be used.
  • the lead frame with a reflector according to the first embodiment of the present invention is a lead frame with a reflector including the reflector having the above-described light reflecting surface, and the light reflecting surface includes the above-described resin, white pigment, and fibrous filler. And a thermal filler / differential thermal analysis based on the TG-DTA method, wherein the fibrous filler has a radial cross-sectional area of 1 ⁇ m 2 or more and 100 ⁇ m 2 or less. After measuring the mass of the reflector before heating using an apparatus, the amount of ash remaining after heating at 600 ° C. for 30 minutes after heating up to 600 ° C.
  • the lead frame with a reflector according to the first embodiment can be manufactured by molding the above-described reflector resin composition into a desired reflector shape by injection molding on the lead frame.
  • the lead frame refers to a substrate on which the reflector is placed. Any lead frame can be used as long as it is used as a substrate in the field of semiconductor light emitting devices.
  • the material for the lead frame include ceramics composed of a sintered body such as alumina, aluminum nitride, mullite, and glass.
  • a resin material having flexibility such as polyimide resin can be used.
  • a reflector substrate made of metal is referred to as a lead frame.
  • the shapes of the terminal portions and the like formed on the lead frame may be formed by half etching.
  • Aluminum, copper, and an alloy of copper are used as the metal material for forming the reflector substrate.
  • it may be plated with a noble metal having a high reflectance such as silver.
  • the thickness of the lead frame with a reflector which concerns on 1st Embodiment is 0.1 mm or more and 3.0 mm or less.
  • the semiconductor light emitting device includes an optical semiconductor element 10 and a reflector 12 provided around the optical semiconductor element 10 and having a light reflecting surface that reflects light from the optical semiconductor element 10 in a predetermined direction. 14 on.
  • the optical semiconductor element 10 is preferably an LED element or an LED package.
  • the reflector 12 corresponds to the above-described reflector, and at least a part (all in the case of FIG. 1) of the light reflecting surface is formed of a molded body made of the above-described reflector resin composition.
  • the optical semiconductor element 10 emits radiated light (generally UV or blue light in a white light LED), for example, an active layer made of AlGaAs, AlGaInP, GaP or GaN sandwiched between n-type and p-type cladding layers. It is a semiconductor chip (light emitter) having a double heterostructure, and has a hexahedral shape with a side length of about 0.5 mm, for example. In the case of wire bonding mounting, it is connected to an electrode (connection terminal) (not shown) via a lead wire 16.
  • radiated light generally UV or blue light in a white light LED
  • an active layer made of AlGaAs, AlGaInP, GaP or GaN sandwiched between n-type and p-type cladding layers.
  • It is a semiconductor chip (light emitter) having a double heterostructure, and has a hexahedral shape with a side length of about 0.5 mm, for example.
  • wire bonding mounting
  • the shape of the reflector 12 conforms to the shape of the end portion (joint portion) of the lens 18 and is usually a cylindrical shape such as a square shape, a circular shape, or an oval shape, or an annular shape.
  • the reflector 12 is a cylindrical body (annular body), and all the end faces of the reflector 12 are in contact with and fixed to the surface of the substrate 14.
  • the inner surface of the reflector 12 may be expanded upward in a tapered shape (see FIG. 1).
  • the reflector 12 can also function as a lens holder when the end portion on the lens 18 side is processed into a shape corresponding to the shape of the lens 18.
  • the reflector 12 may have only the light reflecting surface side as a light reflecting layer 12b made of the resin composition of the present invention.
  • the thickness of the light reflection layer 12b is preferably 500 ⁇ m or less, and more preferably 300 ⁇ m or less, from the viewpoint of reducing the thermal resistance.
  • the member 12a on which the light reflecting layer 12b is formed can be made of a known heat resistant resin.
  • the lens 18 is provided on the reflector 12, but this is usually made of resin, and various structures may be adopted and colored depending on the purpose and application.
  • the space formed by the substrate 14, the reflector 12, and the lens 18 may be a transparent sealing portion, or may be a gap if necessary.
  • This space portion is usually a transparent sealing portion filled with a light-transmitting and insulating material, and the force applied by directly contacting the lead wire 16 in wire bonding mounting and indirectly. Prevents electrical defects caused by the lead wire 16 being disconnected, cut, or short-circuited from the connection portion with the optical semiconductor element 10 and / or the connection portion with the electrode due to applied vibration, impact, etc. can do.
  • the optical semiconductor element 10 can be protected from moisture, dust, etc., and the reliability can be maintained over a long period of time.
  • Examples of the material (transparent sealant composition) that imparts translucency and insulation usually include silicone resins, epoxy silicone resins, epoxy resins, acrylic resins, polyimide resins, polycarbonate resins, and the like. Of these, silicone resins are preferred from the viewpoints of heat resistance, weather resistance, low shrinkage, and discoloration resistance.
  • the resin composition according to the first embodiment is molded into a reflector 12 having a predetermined shape on the substrate 14 by transfer molding, compression molding, injection molding, or the like using a mold having a cavity space having a predetermined shape. To do. It is also called outsert molding because a substrate is placed in a mold and a resin is molded thereon. Thereafter, the separately prepared optical semiconductor element 10 and the electrode are fixed to the substrate 14 with an adhesive or a bonding member, and the LED element and the electrode are connected with the lead wire 16.
  • a transparent sealant composition containing a silicone resin or the like is poured into the recess formed by the substrate 14 and the reflector 12, and cured by heating, drying, or the like to obtain a transparent sealing portion.
  • the lens 18 is disposed on the transparent sealing portion to obtain the semiconductor light emitting device shown in FIG.
  • the composition may be cured.
  • the resin composition for a reflector according to the first embodiment has an effect of improving the sealing property and thus improving the life of the semiconductor element due to excellent adhesion in a molded body obtained by molding the resin composition for a reflector.
  • a reflector with a reflector having a thickness of 3.0 mm or less, preferably 1.0 mm or less, and more preferably 0.8 mm or less, or a reflector for a thin semiconductor light emitting device package.
  • the resin composition according to the second embodiment of the present invention is a resin composition containing an inorganic filler containing a polyolefin resin and a white pigment, wherein the polyolefin resin has a weight average molecular weight of 220,000 to 800,000,
  • the white pigment is a resin composition containing more than 200 parts by mass and not more than 500 parts by mass with respect to 100 parts by mass of the polyolefin resin.
  • polymethylpentene it is preferable to use polymethylpentene.
  • the polymethylpentene has a high melting point of 230 to 240 ° C., does not decompose even at a molding temperature of about 280 ° C., and has excellent chemical resistance and electrical insulation properties. Considering such characteristics, for example, it is a polyolefin resin suitable for use as a reflector of a semiconductor light emitting device.
  • the polymethylpentene resin is preferably a homopolymer of 4-methylpentene-1, but 4-methylpentene-1 and other ⁇ -olefins such as ethylene, propylene, 1-butene, 1-pentene and 1-hexene.
  • It may be a copolymer with olefin and a copolymer mainly composed of 4-methyl-1-pentene.
  • an alkene having 10 to 18 carbon atoms is preferably copolymerized, and an alkene having 16 or more carbon atoms is more preferable.
  • the polyolefin resin used in the resin composition according to the second embodiment needs to have a weight average molecular weight of 220,000 to 800,000.
  • the weight average molecular weight is less than 220,000, cracks are generated in the molded product obtained by molding the resin composition, which is not preferable.
  • a reflector of a semiconductor light emitting device is molded, if a crack occurs, the strength of the reflector is reduced, and the reflector may be destroyed in the reflow process.
  • a weight average molecular weight exceeds 800,000, it becomes difficult to shape
  • the lower limit of the weight average molecular weight is preferably 230,000 or more, more preferably 240,000 or more.
  • the upper limit of the weight average molecular weight is preferably 700,000 or less, more preferably 650,000 or less.
  • the weight average molecular weight is preferably a polystyrene equivalent weight average molecular weight measured by gel permeation chromatography (GPC), but is not limited to this as long as the method can measure the weight average molecular weight with good reproducibility.
  • the weight average molecular weight can be measured by a method exemplified for a material extracted with an appropriate solvent.
  • An inorganic filler containing a white pigment is used for the resin composition according to the second embodiment.
  • the white pigment used in the resin composition of the present invention titanium oxide, zinc sulfide, zinc oxide, barium sulfide, potassium titanate and the like can be used alone or in combination, and titanium oxide is particularly preferable.
  • This white pigment is used for imparting a white color tone to the molded product obtained from the resin composition of the present invention, and in particular by making the color tone highly white, the light reflectance of the molded product. Can be improved.
  • a molded product obtained by molding the resin composition of the present invention and having improved light reflectance of the molded product can be used as a reflector. In particular, when a molded body is used as a reflector, good light reflectance is required, and therefore, it is preferable to use titanium oxide that is easily available and excellent in light reflectance as a white pigment.
  • the average particle size of the white pigment is preferably 0.10 to 0.50 ⁇ m, preferably 0.10 to 0.40 ⁇ m in the primary particle size distribution from the viewpoint of obtaining moldability and obtaining high reflectance. Is more preferably 0.21 to 0.25 ⁇ m.
  • An average particle diameter can be calculated
  • a white pigment can be used as the inorganic filler, or a white pigment and an inorganic filler other than the white pigment can be used in combination.
  • inorganic fillers other than white pigments those usually blended in thermoplastic resin compositions and thermosetting resin compositions such as epoxy resins, acrylic resins and silicone resins can be used alone or in combination. .
  • the cross-sectional shape may be a general round glass fiber or a glass fiber having an irregular cross section such as a flat shape.
  • the glass fiber has a cross-sectional shape in which the minor axis D1 of the cross section is 0.5 to 25 ⁇ m, the major axis D2 is 0.5 to 300 ⁇ m, and the ratio D2 / D1 of D2 to D1 is 1.0 to 30.
  • Glass fibers having an average fiber length of 0.75 to 300 ⁇ m are preferable.
  • This glass fiber is usually called milled fiber, and can be obtained by pulverizing long glass fibers.
  • the average cross-sectional area of the glass fiber 1 ⁇ 100 [mu] m 2, preferably when molding the reflector using a glass fiber is 30 ⁇ 85 .mu.m 2, it is possible to improve the adhesiveness between the substrate.
  • the resin composition according to the second embodiment preferably includes a crosslinking agent. After molding a resin composition containing a crosslinking agent, by irradiating the molded body with an electron beam, better heat resistance can be obtained, and deformation of the resulting molded body due to heat can be prevented. .
  • a crosslinking agent has a saturated or unsaturated ring structure, and at least one of atoms forming at least one ring is an allyl group, a methallyl group, an allyl group via a linking group, and It has a structure formed by bonding to any allylic substituent of a methallyl group via a linking group.
  • the crosslinking agent having such a structure By containing the crosslinking agent having such a structure, it is possible to obtain a resin composition that exhibits good electron beam curability and has excellent heat resistance.
  • the saturated or unsaturated ring structure include a cyclo ring, a hetero ring, and an aromatic ring.
  • the number of atoms forming the ring structure is preferably 3 to 12, more preferably 5 to 8, and still more preferably a 6-membered ring.
  • the molecular weight of the crosslinking agent is preferably 1000 or less, more preferably 500 or less, and further preferably 300 or less. When the molecular weight is 1000 or less, it is possible to prevent the dispersibility in the resin composition from being lowered and to cause an effective crosslinking reaction by electron beam irradiation.
  • the number of ring structures is preferably 1 to 3, more preferably 1 or 2, and further preferably 1.
  • the melting point of the crosslinking agent is preferably not more than the melting point of the polyolefin resin to be used, for example, not more than 200 ° C.
  • the crosslinking agent as described above is excellent in fluidity at the time of molding. Therefore, the molding temperature of the resin composition is lowered to reduce the thermal load, the friction at the time of molding is reduced, or an inorganic containing a white pigment is contained. The filler content can be increased.
  • examples of the linking group in the crosslinking agent include an ester bond, an ether bond, an alkylene group, and a (hetero) arylene group.
  • atoms forming the ring atoms that are not bonded to the allylic substituent are in a state in which hydrogen, oxygen, nitrogen, or the like is bonded, or in a state in which various substituents are bonded.
  • the crosslinking agent used in the second embodiment it is preferable that at least two atoms among atoms forming one ring of the crosslinking agent are independently bonded to an allylic substituent.
  • the ring structure is a 6-membered ring, at least two of the atoms forming the ring are independently bonded to an allylic substituent, and one allylic substituent is bonded to the atom.
  • another allylic substituent is bonded to the atom at the meta position.
  • the crosslinking agent is preferably represented by the following formula (1) or (2).
  • R 1 to R 3 are each independently an allylic substituent of any one of an allyl group, a methallyl group, an allyl group via an ester bond, and a methallyl group via an ester bond.
  • R 1 to R 3 are each independently an allylic substituent of any one of an allyl group, a methallyl group, an allyl group via an ester bond, and a methallyl group via an ester bond.
  • crosslinking agent represented by the above formula (1) examples include triallyl isocyanurate, methyl diallyl isocyanurate, diallyl monoglycidyl isocyanuric acid, monoallyl diglycidyl isocyanurate, and trimethallyl isocyanurate.
  • crosslinking agent represented by the above formula (2) examples include orthophthalic acid diallyl ester, isophthalic acid diallyl ester, and the like.
  • a white pigment content rate needs to contain more than 200 mass parts and 500 mass parts or less with respect to 100 mass parts of polyolefin resin.
  • the white pigment content is 200 parts by mass or less, it becomes difficult to make the color tone of the molded product obtained from the resin composition of the second embodiment white, and the light reflectance decreases or the light rays The long-term heat resistance of the reflectivity may decrease, which is not preferable.
  • the white pigment content exceeds 500 parts by mass, it is difficult to make the resin composition into a molded body, which is not preferable.
  • the white pigment content is preferably 300 to 480 parts by mass, more preferably 350 to 450 parts by mass with respect to 100 parts by mass of the polyolefin resin.
  • the inorganic filler other than the white pigment is 10 to 300 parts by mass, preferably 30 to 200 parts by mass, more preferably 50 to 180 parts by mass. If the content of the inorganic filler and the white pigment is within the above range, the color tone of the resulting molded product can be highly white, and when the molded product is a reflector, the light reflectance can be improved, And the dimensional stability of a molded object can be made excellent.
  • the content of the inorganic filler including the white pigment in the resin composition according to the second embodiment is 70 to 90% by mass, preferably 72 to 88% by mass, and more preferably 75 to 85% by mass. Is desirable.
  • the content of the inorganic filler containing the white pigment in the resin composition according to the second embodiment can be measured as the ash content.
  • the method for measuring the ash content contained in the resin composition according to the second embodiment includes a method (JIS K 7250-1 (ISO 3451-1)) defined as a general method for obtaining the ash content of a resin composition, and It can be measured according to a compliant method or a TG-DTA method.
  • JIS K 7250-1 ISO 3451-1
  • a method based thereon it is preferable to measure by JIS K 7250-1 (ISO 3451-1) and a method based thereon.
  • JIS K 7250-1 (ISO 3451-1) and the method based thereon require a very large amount of sample, if a sufficient amount of sample cannot be obtained, the TG-DTA method can be used. Good.
  • the measurement conditions for ash are described below.
  • the ash content in the resin composition according to the second embodiment can be accurately measured by the measurement method described above, but the inorganic filler containing a white pigment with respect to the total amount of the resin composition It can also be calculated roughly from the proportion of the amount.
  • the polyolefin resin content in the resin composition of the second embodiment is 7 to 30% by mass, preferably 11 to 28% by mass.
  • the cross-linking agent can be used, and the content of the cross-linking agent is 15 to 40 parts by mass, preferably 15 to 100 parts by mass of the polyolefin resin. It is desirable to contain an amount of ⁇ 30 parts by mass, more preferably 16 to 20 parts by mass. If the crosslinking agent is within the above range, crosslinking can be carried out effectively without bleeding out the crosslinking agent from the molded product before crosslinking.
  • the resin composition according to the second embodiment can contain various additives as long as the effects of the present invention are not impaired.
  • Additives can be blended.
  • a dispersant such as a silane coupling agent can be blended with the resin composition according to the second embodiment.
  • the silane coupling agent include disilazane such as hexamethyldisilazane; cyclic silazane; trimethylsilane, trimethylchlorosilane, dimethyldichlorosilane, methyltrichlorosilane, allyldimethylchlorosilane, trimethoxysilane, benzyldimethylchlorosilane, Methyltrimethoxysilane, methyltriethoxysilane, isobutyltrimethoxysilane, dimethyldimethoxysilane, dimethyldiethoxysilane, trimethylmethoxysilane, hydroxypropyltrimethoxysilane, phenyltrimethoxysilane, n-butyltrimethoxysilane, n-hexadecyl Trimethoxysilane,
  • the resin composition according to the second embodiment is prepared by melting and kneading the above-described inorganic filler containing the polyolefin resin and the white pigment and the crosslinking agent preferably used in the above-described content ratio, and the like. Can be produced as a granulated product.
  • a known melt-kneading method such as a melt-kneading extruder, a two-roll or three-roll, a stirrer such as a homogenizer or a planetary mixer, or a melt-kneader such as a polylab system or a lab plast mill is used. be able to.
  • the molded body obtained from the resin composition according to the second embodiment is free from cracks, has excellent heat resistance, and has a white color tone. Therefore, it can be applied to various applications. For example, it can be applied as a heat-resistant insulating film, a heat-resistant release sheet, a light-reflecting sheet for solar cells, a reflector for a light source for televisions, or a light source for television.
  • the sealing performance of the optical semiconductor element affects the element life. For this reason, the resin composition for reflectors and the reflector obtained from the resin composition according to the second embodiment are less likely to generate cracks and have high sealing properties, and thus can be preferably applied to LEDs.
  • a metal substrate type LED which is manufactured by processing a lead frame by etching and half-etching and uses the back surface of the element installation portion as an electrode.
  • molding methods such as transfer molding, compression molding, and injection molding can be used.
  • an injection molding method it can be obtained by injection molding at a cylinder temperature of 200 to 400 ° C. and a mold temperature of 20 to 150 ° C.
  • the resin composition using a crosslinking agent it can obtain by performing an electron beam irradiation process to the obtained molded object.
  • the electron beam irradiation treatment can be performed on a resin composition using a crosslinking agent, and the resin composition subjected to the electron beam irradiation treatment can be molded to obtain a molded body.
  • the acceleration voltage of an electron beam it can select suitably according to the magnitude
  • the crosslinking agent used can be crosslinked and cured at an acceleration voltage of about 250 to 3000 kV.
  • the transmission capability increases as the acceleration voltage increases. Therefore, when using a base material that deteriorates due to the electron beam as the base material, the transmission depth of the electron beam and the thickness of the molded body are substantially equal.
  • the accelerating voltage so as to be equal to each other, it is possible to suppress irradiation of an excessive electron beam to the molded body, and to minimize degradation of the molded body due to excess electron beams.
  • the absorbed dose when irradiating with an electron beam is appropriately set depending on the composition of the resin composition, but the amount at which the crosslink density in the molded body is saturated is preferable, and the irradiated dose is preferably 50 to 600 kGy.
  • the electron beam source is not particularly limited.
  • various electron beam accelerators such as a cockroft Walton type, a bandegraft type, a resonant transformer type, an insulated core transformer type, a linear type, a dynamitron type, and a high frequency type. Can be used.
  • the reflector according to the second embodiment of the present invention is formed by molding the above-described resin composition of the present invention.
  • the reflector may be used in combination with a semiconductor light-emitting device to be described later, or may be used in combination with a semiconductor light-emitting device (LED mounting substrate) made of another material.
  • the reflector according to the second embodiment mainly has an action of reflecting light from the LED element of the semiconductor light emitting device toward the lens (light emitting portion).
  • the details of the reflector are the same as those of the reflector (reflector 12 described later) applied to the semiconductor light emitting device of the present invention, and are omitted here.
  • the molded object obtained from the resin composition which concerns on 2nd Embodiment does not generate
  • the lead frame with a reflector according to the second embodiment is formed by molding the resin composition according to the second embodiment described above.
  • the lead frame indicates a substrate on which the reflector is placed.
  • Any lead frame can be used as long as it is used in the field of semiconductor light emitting devices.
  • the material of the lead frame include ceramics made of a sintered body such as alumina, aluminum nitride, mullite, and glass.
  • a resin material having flexibility such as polyimide resin can be used.
  • a lead frame made of metal is often made of aluminum, copper, or an alloy of copper, and is often plated with a noble metal having a high reflectance such as silver in order to improve the reflectance.
  • a reflector substrate made of metal is often called a lead frame. Terminal portions and the like formed on the lead frame may be formed by half etching.
  • the lead frame with a reflector according to the second embodiment is manufactured by molding the resin composition according to the second embodiment on the above-described lead frame into a desired reflector shape.
  • the thickness of the lead frame with reflector according to the second embodiment is preferably 0.1 to 3.0 mm, more preferably 0.1 to 1.0 mm, More preferably, it is ⁇ 0.8 mm.
  • the lead frame with a reflector according to the second embodiment is to be a semiconductor light emitting device by mounting an LED chip on the reflector, further sealing with a known sealing agent, and die bonding to obtain a desired shape. Can do.
  • the lead frame with a reflector of this invention acts as a reflector, it is functioning also as a frame which supports a semiconductor light-emitting device.
  • semiconductor light emitting device An example of the semiconductor light emitting device and the manufacturing method thereof according to the second embodiment can be configured in the same manner as the semiconductor light emitting device described with reference to FIGS. 1 and 2 described above.
  • Example according to First Embodiment A reflector according to the first embodiment will be described in detail using an example.
  • the first invention is not limited to these examples.
  • [Resin composition for reflector] The resin compositions for reflectors of Examples and Comparative Examples were prepared by the following methods, and the moldability and ash content were evaluated. The results are shown in Table 1. ⁇ Preparation of resin composition for reflector> The following various materials are mixed by using an extruder (Nippon Placon Co., Ltd. MAX30: die diameter: 3.0 mm) and a pelletizer (Toyo Seiki Co., Ltd., MPPEC1) according to the formulation shown in Table 1, and a resin composition for reflectors. I got a thing.
  • White pigment Titanium oxide particles: average particle size 0.21 ⁇ m
  • Fibrous filler 1 Glass fiber: PF70E-001 (manufactured by Nittobo Co., Ltd., average fiber length 62 ⁇ m, average cross-sectional area 104.2 ⁇ m 2 , and cross-sectional shape is round glass fiber) Fiber filler 2 ...
  • glass fiber SS05DE-413SP (manufactured by Nittobo Co., Ltd., average fiber length 65 ⁇ m, average cross-sectional area 41.6 ⁇ m 2 , cross-sectional shape is round glass fiber)
  • Fibrous filler 3 Glass fiber: EFDE50-01 (manufactured by Central Glass Fiber Co., Ltd., average fiber length 55 ⁇ m, average cross-sectional area 33.2 ⁇ m 2 ) -Fibrous filler 4 ...
  • glass fiber MF03JB1-20 (Asahi Fiber Glass Co., Ltd., average fiber length 71 ⁇ m, average cross-sectional area 81.7 ⁇ m 2 ) ⁇
  • Crosslinking agent ... triallyl isocyanurate ⁇ Silane coupling agent ... Hexyltrimethoxysilane ⁇ Antioxidant 1 ...
  • IRGANOX1010 manufactured by BASF Japan Ltd.
  • Antioxidant 2 ⁇ Bis (2,6-di-tert-butyl-4-methylphenyl) pentaerythritol diphosphite
  • Mold release agent ⁇ Zinc stearate
  • the average fiber The length and average cross-sectional area were measured by fixing the sample before mixing with the reflector resin composition on a sample stage for SEM observation using carbon tape, and observing it with SEM (Hitachi High-Technologies S-4800). Value. It calculated as an average value of at least 10 fibrous fillers.
  • ⁇ Pellet creation> The step of obtaining the resin composition is kneaded using an extruder screw. If a resin composition stably pelletized is obtained in this step, the load applied to the screw of the extruder is acceptable. The case where a resin composition that is large and cannot be continuously operated and cannot be stably pelletized cannot be obtained.
  • a lead frame with a reflector was produced using the resin composition for a reflector under the following conditions.
  • a resin composition (thickness: 700 ⁇ m, external dimensions: 35 mm ⁇ 35 mm, opening: 2.9 mm ⁇ 2.9 mm) is applied to a silver plating frame (thickness: 250 ⁇ m).
  • the lead frame with the reflector was obtained by molding.
  • the injection molding machine conditions were as follows: cylinder temperature: 270 ° C., mold temperature: 80 ° C., injection speed: 100 mm / sec, holding pressure: 80 MPa, holding pressure time: 1 sec, cooling time: 8 sec.
  • This molded product was cured by irradiation with an electron beam at an acceleration voltage of 800 kV and an irradiation dose of 400 kGy to obtain a cured resin composition for a reflector.
  • ⁇ Heat deformation temperature> The specimen was compliant with ASTM D648, and the temperature at which the specified deflection amount was reached was defined as the deflection temperature under load (thermal deformation temperature).
  • the lead frame with a reflector of an Example and a comparative example was produced with the following method, and adhesiveness, a reflectance, and durability A were evaluated. The results are shown in Table 1.
  • ⁇ Production of lead frame with reflector> The following evaluation is performed by molding a resin composition for a reflector produced under the same conditions as those used for the above-described evaluation of moldability, and curing by applying an electron beam at an acceleration voltage of 800 kV and an irradiation dose of 400 kGy. A lead frame was obtained.
  • ⁇ Adhesion> The degree of adhesion between each specimen of the lead frame with a reflector and the substrate was measured by a red check test to determine whether or not it was possible.
  • ⁇ Durability A> The reflectance was measured after the specimen of the lead frame with a reflector was left at 200 ° C. for 45 hours. The reflectance was measured using the reflectance measuring apparatus under the same conditions. Comparison was made at a reflectance of a wavelength of 450 nm.
  • a light emitting device was manufactured using the lead frames with reflectors of Examples and Comparative Examples, and the initial luminous flux was evaluated. The results are shown in Table 1.
  • the reflector resin composition produced by the formulation shown in Table 1 was molded into a reflector shape, and the molded body was cured by irradiation with an electron beam at an acceleration voltage of 800 kV and an irradiation dose of 400 kGy.
  • a lead frame with a reflector was obtained after curing.
  • the obtained lead frame with reflector and the separately prepared LED element and electrode are fixed on the substrate with an adhesive, and the LED element and the electrode are connected with a lead wire, then diced into individual pieces, and a semiconductor light emitting device ( LED package) was obtained.
  • Solder was provided on the wiring board, the semiconductor light emitting device was placed on the solder, heated to 240 ° C. in a reflow furnace, the solder was melted, and the semiconductor light emitting device was mounted on the wiring board.
  • the cross-sectional area of the fibrous filler was measured as follows.
  • the reflector of the semiconductor light emitting device was broken, and the fractured surface was observed with SEM (Hitachi High-Technologies S-4800). After fixing the fracture surface to a metal sample stage in parallel, the fracture surface was observed at a magnification of 2500 from the direction perpendicular to the fracture surface.
  • the diameter length of the fibrous filler appearing in the cross section of the reflector was measured.
  • the cross section of the filler was elliptical, the major axis and minor axis of the ellipse were measured and the ratio of major axis to minor axis was 0.8 to 1.2.
  • the diameter was measured up to 3 significant figures.
  • the cross-sectional area was computed as an average value about the thing of 50% of the total number of measurements from a thing with a small cross-sectional area among the cross sections of a fibrous filler. Sampling was performed to obtain an average value of at least 10 cross sections. That is, if the total number of measurements was 20, the average value for 10 was calculated from the one with the smallest cross-sectional area. The third digit of the numerical value after calculation was rounded off to obtain the cross-sectional area value.
  • Example 1 As shown in Table 1, it was found that the one using the reflector resin composition prepared by the formulation of Example 1-4 can improve the adhesion without impairing the characteristics required for the production of the light emitting device. It was. In particular, the larger the cross-sectional size of the fibrous filler, the better the reflectance. When the fibrous filler having a cross-sectional area of 81.7 ⁇ m 2 was used, both the reflectance and the durability A could be remarkably improved as compared with the comparative example. In Comparative Example 3, Comparative Example 4, and Comparative Example 5 in which the ash content is 70% or less, the durability A is remarkably deteriorated, and use in a light emitting device is not preferable. On the other hand, Comparative Example 6 could not be used as a reflector resin composition because a resin composition used for molding could not be obtained.
  • Example according to Second Embodiment A reflector according to the second embodiment will be described in detail using an example.
  • the second invention is not limited to these examples.
  • the materials used in Examples 11 to 25 and Comparative Examples 11 to 13 are as follows.
  • White pigment / titanium oxide particles PF-691 (Ishihara Sangyo Co., Ltd. Rutile structure average particle size 0.21 ⁇ m)
  • Inorganic filler / glass fiber other than white pigment PF70E-001 (manufactured by Nittobo Co., Ltd., fiber length 70 ⁇ m, average cross-sectional area 95.0 ⁇ m 2 , cross-sectional shape is glass fiber)
  • Crosslinking agent 1 (triallyl isocyanurate) manufactured by Nippon Kasei Co., Ltd.
  • Crosslinking agent 2 MeDAIC (methyldiallyl isocyanurate) Shikoku Kasei Kogyo Co., Ltd.
  • Crosslinking agent 3 DA-MGIC diallyl monoglycidyl isocyanuric acid
  • Cross-linking treatment agent 4 manufactured by Shikoku Kasei Kogyo Co., Ltd.
  • MA-DGIC monoallyl diglycidyl isocyanurate
  • TMAIC trimethallyl isocyanurate
  • Crosslinking agent 6 DUP monomer diallyl ester of orthophthalic acid
  • Silane coupling agent Hexyltrimethoxysilane [KBM-3063 (Shin-Etsu Chemical Co., Ltd.)] Release agent: Zinc stearate [SZ-2000 (manufactured by Sakai Chemical Co., Ltd.)]
  • the resin composition (pellet) obtained above is used on an injection molding machine Sodick TR40ER Sodick (prep plastic type) on a silver plating frame (lead frame) (thickness: 250 ⁇ m), thickness: 700 ⁇ m, external dimensions: 35 mm.
  • a lead frame (2) with a reflector was obtained by molding so as to have a size of ⁇ 35 mm and an opening: 2.9 mm ⁇ 2.9 mm.
  • the lead frame with reflector (2) has 36 openings.
  • the injection molding machine conditions were as follows: cylinder temperature: 260 ° C., mold temperature: 70 ° C., injection speed: 200 mm / sec, holding pressure: 100 MPa, holding pressure time: 1 sec, cooling time: 15 sec.
  • These compacts (1) and (2) were irradiated with an electron beam at an acceleration voltage of 800 kV and an absorbed dose of 400 kGy. The following characteristics were evaluated. The results are shown in Tables 2 to 5 below.
  • MFR of the resin composition was measured by a method based on the method described in MFR of JIS K 7210: 1999 thermoplastics. Specifically, the test is performed at a test temperature of 280 ° C., a test load of 2.16 kg, and 60 seconds. As a measuring device, a melt flow tester manufactured by Thiast Co. was used. The MFR is shown in Tables 2-5.
  • a resin composition containing an inorganic filler containing a polyolefin resin and a white pigment wherein the polyolefin resin has a weight average molecular weight of 220,000 to 800,000, and contains a white pigment
  • the resin composition having a rate of more than 200 parts by mass and less than 500 parts by mass with respect to 100 parts by mass of the polyolefin resin yields a molded body having less heat cracking on the surface and excellent heat resistance in reflectance. be able to.
  • Table 5 it can be seen that when a polyolefin resin having a weight average molecular weight of less than 220,000 is used, generation of cracks increases on the surface of the molded body.
  • the content of the white pigment is less than 200 parts by mass, and after 35 hours at 200 ° C. It has been shown that the reflectance of the film is greatly reduced and the heat resistance is poor. From the above, it can be said that the resin composition of the present invention is useful for reflectors and reflectors for semiconductor light emitting devices.

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  • Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Compositions Of Macromolecular Compounds (AREA)

Abstract

La présente invention porte sur un réflecteur comportant une surface réfléchissant la lumière qui est constitué d'une composition de résine contenant une résine et une charge inorganique incluant un pigment blanc et une charge fibreuse. L'aire de section transversale dans la direction radiale de ladite charge fibreuse est comprise entre 1 et 100 µm2 inclus. Au moyen d'un analyseur thermogravimétrique/thermique différentiel simultané sur la base d'un procédé TG/DTA, la masse dudit réflecteur avant chauffage est mesurée, puis la teneur de cendre résiduelle est mesurée après le chauffage dudit réflecteur, dans l'atmosphère ambiante, à 600 °C à 10 °C/min, puis pendant 30 minutes à 600 °C. Puisque la teneur mesurée de cendre résiduelle est comprise entre 70 et 90 % en masse inclus, sur la base de la masse totale dudit réflecteur avant chauffage, la présente invention peut assurer une excellente adhésion du réflecteur à un substrat tout en maintenant au moins une performance de base, par exemple des besoins de résistance à la chaleur et de réflectivité.
PCT/JP2015/071880 2014-08-01 2015-07-31 Réflecteur et composition de résine Ceased WO2016017818A1 (fr)

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JP2010080793A (ja) * 2008-09-26 2010-04-08 Toyoda Gosei Co Ltd 光反射部材及び発光装置
JP2012229390A (ja) * 2010-10-22 2012-11-22 Panasonic Electric Works Co Ltd Ｌｅｄリフレクター用不飽和ポリエステル樹脂組成物及びこれを用いたｌｅｄリフレクター、ｌｅｄ照明器具
JP2013166926A (ja) * 2012-01-17 2013-08-29 Dainippon Printing Co Ltd 電子線硬化性樹脂組成物、リフレクター用樹脂フレーム、リフレクター、半導体発光装置、及び成形体の製造方法

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WO2007037355A1 (fr) * 2005-09-30 2007-04-05 Nichia Corporation Dispositif élecroluminescent et unité rétro-eclairante utilisant ledit dispositif électroluminescent
JP2008078638A (ja) * 2006-08-22 2008-04-03 Mitsubishi Chemicals Corp 半導体デバイス用部材、並びに半導体デバイス用部材形成液及び半導体デバイス用部材の製造方法、並びに、それを用いた半導体発光デバイス、半導体デバイス用部材形成液、及び蛍光体組成物
JP2010080793A (ja) * 2008-09-26 2010-04-08 Toyoda Gosei Co Ltd 光反射部材及び発光装置
JP2012229390A (ja) * 2010-10-22 2012-11-22 Panasonic Electric Works Co Ltd Ｌｅｄリフレクター用不飽和ポリエステル樹脂組成物及びこれを用いたｌｅｄリフレクター、ｌｅｄ照明器具
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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2018160654A (ja) * 2016-07-19 2018-10-11 パナソニックＩｐマネジメント株式会社 光反射体、ベース体、発光装置及びベース体の製造方法
JP7065381B2 (ja) 2016-07-19 2022-05-12 パナソニックＩｐマネジメント株式会社 光反射体、ベース体、発光装置及びベース体の製造方法

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