WO2013047606A1 - 表面実装型発光装置用樹脂成形体およびその製造方法ならびに表面実装型発光装置 - Google Patents
表面実装型発光装置用樹脂成形体およびその製造方法ならびに表面実装型発光装置 Download PDFInfo
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- WO2013047606A1 WO2013047606A1 PCT/JP2012/074757 JP2012074757W WO2013047606A1 WO 2013047606 A1 WO2013047606 A1 WO 2013047606A1 JP 2012074757 W JP2012074757 W JP 2012074757W WO 2013047606 A1 WO2013047606 A1 WO 2013047606A1
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- POSICDHOUBKJKP-UHFFFAOYSA-N prop-2-enoxybenzene Chemical compound C=CCOC1=CC=CC=C1 POSICDHOUBKJKP-UHFFFAOYSA-N 0.000 description 1
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- FBCQUCJYYPMKRO-UHFFFAOYSA-N prop-2-enyl 2-methylprop-2-enoate Chemical compound CC(=C)C(=O)OCC=C FBCQUCJYYPMKRO-UHFFFAOYSA-N 0.000 description 1
- CAEWJEXPFKNBQL-UHFFFAOYSA-N prop-2-enyl carbonochloridate Chemical compound ClC(=O)OCC=C CAEWJEXPFKNBQL-UHFFFAOYSA-N 0.000 description 1
- QTECDUFMBMSHKR-UHFFFAOYSA-N prop-2-enyl prop-2-enoate Chemical compound C=CCOC(=O)C=C QTECDUFMBMSHKR-UHFFFAOYSA-N 0.000 description 1
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- JIYNFFGKZCOPKN-UHFFFAOYSA-N sbb061129 Chemical class O=C1OC(=O)C2C1C1C=C(C)C2C1 JIYNFFGKZCOPKN-UHFFFAOYSA-N 0.000 description 1
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- 238000000926 separation method Methods 0.000 description 1
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- MHFJYSOKRPQWNF-UHFFFAOYSA-N silane triethoxy-[2-(7-oxabicyclo[4.1.0]heptan-3-yl)ethyl]silane Chemical class [SiH4].CCO[Si](CCC1CCC2OC2C1)(OCC)OCC MHFJYSOKRPQWNF-UHFFFAOYSA-N 0.000 description 1
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- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 description 1
- HKZLPVFGJNLROG-UHFFFAOYSA-M silver monochloride Chemical compound [Cl-].[Ag+] HKZLPVFGJNLROG-UHFFFAOYSA-M 0.000 description 1
- RYYKJJJTJZKILX-UHFFFAOYSA-M sodium octadecanoate Chemical compound [Na+].CCCCCCCCCCCCCCCCCC([O-])=O RYYKJJJTJZKILX-UHFFFAOYSA-M 0.000 description 1
- NTHWMYGWWRZVTN-UHFFFAOYSA-N sodium silicate Chemical compound [Na+].[Na+].[O-][Si]([O-])=O NTHWMYGWWRZVTN-UHFFFAOYSA-N 0.000 description 1
- NTVDGBKMGBRCKB-UHFFFAOYSA-M sodium;12-hydroxyoctadecanoate Chemical compound [Na+].CCCCCCC(O)CCCCCCCCCCC([O-])=O NTVDGBKMGBRCKB-UHFFFAOYSA-M 0.000 description 1
- VYPDUQYOLCLEGS-UHFFFAOYSA-M sodium;2-ethylhexanoate Chemical compound [Na+].CCCCC(CC)C([O-])=O VYPDUQYOLCLEGS-UHFFFAOYSA-M 0.000 description 1
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- JDLYKQWJXAQNNS-UHFFFAOYSA-L zinc;dibenzoate Chemical compound [Zn+2].[O-]C(=O)C1=CC=CC=C1.[O-]C(=O)C1=CC=CC=C1 JDLYKQWJXAQNNS-UHFFFAOYSA-L 0.000 description 1
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- DRDVZXDWVBGGMH-UHFFFAOYSA-N zinc;sulfide Chemical compound [S-2].[Zn+2] DRDVZXDWVBGGMH-UHFFFAOYSA-N 0.000 description 1
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- GFQYVLUOOAAOGM-UHFFFAOYSA-N zirconium(iv) silicate Chemical compound [Zr+4].[O-][Si]([O-])([O-])[O-] GFQYVLUOOAAOGM-UHFFFAOYSA-N 0.000 description 1
Images
Classifications
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- 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
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- 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
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- B29C45/00—Injection moulding, i.e. forcing the required volume of moulding material through a nozzle into a closed mould; Apparatus therefor
- B29C45/14—Injection moulding, i.e. forcing the required volume of moulding material through a nozzle into a closed mould; Apparatus therefor incorporating preformed parts or layers, e.g. injection moulding around inserts or for coating articles
- B29C45/14639—Injection moulding, i.e. forcing the required volume of moulding material through a nozzle into a closed mould; Apparatus therefor incorporating preformed parts or layers, e.g. injection moulding around inserts or for coating articles for obtaining an insulating effect, e.g. for electrical components
- B29C45/14655—Injection moulding, i.e. forcing the required volume of moulding material through a nozzle into a closed mould; Apparatus therefor incorporating preformed parts or layers, e.g. injection moulding around inserts or for coating articles for obtaining an insulating effect, e.g. for electrical components connected to or mounted on a carrier, e.g. lead frame
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- B29C45/00—Injection moulding, i.e. forcing the required volume of moulding material through a nozzle into a closed mould; Apparatus therefor
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- B29C45/372—Mould cavity walls, i.e. the inner surface forming the mould cavity, e.g. linings provided with means for marking or patterning, e.g. numbering articles
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/24—Structurally defined web or sheet [e.g., overall dimension, etc.]
- Y10T428/24802—Discontinuous or differential coating, impregnation or bond [e.g., artwork, printing, retouched photograph, etc.]
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/24—Structurally defined web or sheet [e.g., overall dimension, etc.]
- Y10T428/24802—Discontinuous or differential coating, impregnation or bond [e.g., artwork, printing, retouched photograph, etc.]
- Y10T428/24851—Intermediate layer is discontinuous or differential
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/24—Structurally defined web or sheet [e.g., overall dimension, etc.]
- Y10T428/24802—Discontinuous or differential coating, impregnation or bond [e.g., artwork, printing, retouched photograph, etc.]
- Y10T428/24917—Discontinuous or differential coating, impregnation or bond [e.g., artwork, printing, retouched photograph, etc.] including metal layer
Definitions
- the present invention relates to a resin molded body for a surface-mounted light-emitting device, a manufacturing method thereof, and a surface-mounted light-emitting device.
- Surface-mount light-emitting devices equipped with light-emitting elements such as light-emitting diodes (LEDs) and laser diodes (LDs) can produce high-luminance light with excellent visibility, and can be miniaturized and consumed. It has many advantages such as low power and long life. For this reason, surface-mounted light-emitting devices are used, for example, as light sources such as light bulbs, downlights, base lights, street lights, traffic lights, and backlight sources such as liquid crystal displays, and their applications are rapidly expanding.
- a typical surface-mounted light-emitting device includes, for example, a resin molded body having a lead frame disposed so that a pair of leads are spaced apart from each other, a recess in which the lead frame is exposed at the bottom, and an insulating portion that insulates the pair of leads. And a light emitting element mounted on a lead frame exposed at the bottom of the recess and connected to the pair of leads so as to be energized, and a transparent resin layer formed by filling the recess with a transparent resin (Patent Document) 1 and 2).
- the resin molded body has a function of protecting the light emitting element and reflecting light emitted from the light emitting element toward the front surface of the light emitting device to increase luminance.
- Ag used as a plating layer on the lead frame surface exhibits the highest light reflectance among metals, and is therefore suitable as a material for the reflective film in order to reflect a large amount of light.
- Ag reacts with the halogen ions and sulfur contained in the atmosphere and the sealing resin as the usage time of the surface-mounted light-emitting device elapses, thereby causing a halide such as chloride (AgCl) or sulfide (Ag 2 S).
- a halide such as chloride (AgCl) or sulfide (Ag 2 S).
- Ag has a characteristic of aggregating with heat generated from the light emitting element, and this characteristic also has a problem of reducing the light reflectance.
- Patent Document 3 discloses that an Ag—Au alloy plating in which a silicone resin is applied as a sealing resin and chloride or sulfide is difficult to form on a pure Ag plating layer on a reflective surface.
- a lead frame is described which is further coated with layers.
- the Ag—Au alloy plating layer is made of an alloy containing Au as a main component with an Ag content limited to less than 50% by mass, the forming operation is complicated, and the thickness is 0.1 ⁇ m or more and 0.0. Since it is 6 micrometers or less, cost also becomes high.
- the surface-mounted light-emitting device is manufactured by, for example, transfer molding using a thermosetting resin as a resin material that gives a resin molded body. More specifically, an upper mold having an upper mating surface in which a recess corresponding to the three-dimensional shape of the resin molded body is formed at a predetermined position, a lower mold having a flat lower mating surface, a resin injection hole, A surface-mount light-emitting device is manufactured by a method including the following steps (a) to (f) using a mold including: (see Patent Documents 1 and 4).
- a step of sandwiching and fixing the lead frame between the upper mating surface and the lower mating surface (B) A step of injecting a liquid thermosetting resin from the resin injection hole into the internal space formed by the concave portion of the upper mating surface and the lead frame and / or the lower mating surface. (C) A step of curing the injected liquid thermosetting resin by heating the mold and bonding the resin cured body to a predetermined position of the lead frame. (D) A step of removing the mold and obtaining a resin molded body in which the lead frame and the cured resin body are integrally molded, and the bottom portion has a recess in which the lead frame is exposed. (E) A step of mounting the light emitting element on the lead frame exposed at the bottom of the recess so as to be energized. (F) A step of sealing the light emitting element by filling the concave portion with a transparent resin.
- the above-described conventional manufacturing method has an advantage that a large number of surface-mounted light-emitting devices can be manufactured at a time by using transfer molding.
- the demolding step (d) since the mold release property of the resin molded body from the mold is very poor, the resin molded body is likely to be deformed. In some cases, cohesive failure occurs, and the resin molded body is destroyed. There is a problem of being. Therefore, in the conventional manufacturing method, the defective product rate may be very high.
- the object of the present invention is a surface mount type that is excellent in releasability from a mold, is less likely to be deformed, resin chipped or coherently broken when the mold is removed, and further prevents adhesion of resin burrs to the lead frame portion. It is an object to provide a resin molded body for a light emitting device, a method for producing the same, and a surface-mounted light emitting device using the same.
- the present inventors have adjusted the ten-point average roughness (Rz) of the bottom surface of the upper recess formed on the upper mating surface of the upper mold to a specific range.
- Rz ten-point average roughness
- the present inventors efficiently mass-produce resin molded bodies having substantially the same three-dimensional shape by carrying out transfer mold molding using a mold including an upper mold having such an upper recess. I found out that I can do it. The present inventors have completed the present invention based on these findings.
- the present invention provides the following resin molded product for a surface-mounted light-emitting device, a method for producing the same, and a surface-mounted light-emitting device using the resin molded product.
- a resin-molded body for a surface-mounted light-emitting device in which a cured resin body and a plurality of leads are integrally molded, and a plurality of leads are exposed at the bottom, the ten-point average roughness (Rz) of the opening surface of the recess Is 1 ⁇ m or more and 10 ⁇ m or less, the glass transition temperature of the cured resin is 10 ° C. or more, the glass transition temperature is ⁇ 50 to 250 ° C.
- thermomechanical analyzer TMA
- the heating rate is 5 It was a value measured under the conditions of ° C / min and a sample size length of 1 to 5 mm, and the light reflectance at 460 nm of the opening surface of the recess was 80% or more, and the resin molded body was heated at 180 ° C for 72 hours.
- a resin-molded body for a surface-mounted light-emitting device having a light reflectance retention of 90% or more at a later opening surface.
- the resin cured product contains (A) an organic compound containing at least two carbon-carbon double bonds reactive with SiH groups in one molecule, and (B) containing at least two SiH groups in one molecule.
- At least one of the plurality of leads has a metal layer on the surface, the metal layer has an outermost surface layer on the surface side, and the outermost surface layer is an Au layer having a thickness of 0.003 to 0.05 ⁇ m, an Au-based alloy layer 4.
- the metal layer has an outermost surface layer and a second metal layer interposed between the surface of the lead and the outermost surface layer.
- the second metal layer includes an Ag layer, a Pd layer, or an Ag layer and a Pd layer. 5.
- the recess has a bottom surface that is the surface of the plurality of leads exposed at the bottom, and the inner wall surface of the recess rises from the periphery of the bottom surface continuously to the bottom surface, and has an inclination angle of 45 ° to 90 ° with respect to the bottom surface.
- Two slopes a first slope that rises from the periphery of the second slope toward the opening surface continuously to the second slope, and has an inclination angle with respect to the bottom surface that is greater than 0 ° and equal to or less than 45 °, 7.
- the resin-molded body for a surface-mounted light-emitting device according to any one of 1 to 6 above, wherein the boundary with the second slope is located at a position that is higher than 0 ⁇ m and 100 ⁇ m or less from the bottom surface of the inner wall surface of the recess.
- the plurality of leads include a first lead and a second lead arranged so as to be separated from each other, and the resin cured body has an insulating portion interposed between the first lead and the second lead to insulate them.
- the resin-molded body for a surface-mounted light-emitting device according to any one of 1 to 7 above, wherein the insulating portion is exposed at the bottom of the recess while being sandwiched between the first lead and the second lead.
- the first lead includes a first inner lead portion exposed at the bottom of the recess and a first outer lead portion that contacts the resin cured body, and the second lead is a second inner lead exposed at the bottom of the recess.
- the resin-molded body for a surface-mounted light-emitting device according to 8 above including a portion and a second outer lead portion that contacts the cured resin body. 10. 10. The resin molded body for a surface-mounted light-emitting device according to 9 above, wherein the first outer lead portion and / or the second outer lead portion are exposed on the outer surface.
- the cured resin and the plurality of leads are integrally formed, and the bottom has a recess where the plurality of leads are exposed, and the ten-point average roughness (Rz) of the opening surface of the recess in the cured resin body is 0.5 ⁇ m or more and 15 ⁇ m.
- a method for producing a resin molded body for a surface-mounted light-emitting device which is the following: (1) having an internal space corresponding to the three-dimensional shape of a cured resin body, and having a 10-point average roughness (Rz) of the bottom surface of 1 ⁇ m or more An upper mold having an upper mating surface in which an upper concave portion of 10 ⁇ m or less is formed at a predetermined position, a lower mold having a flat lower mating surface, and a resin injection hole is used.
- a method for producing a resin molded body for a surface-mounted light emitting device comprising: a step of producing an integrally molded resin molded body; and (4) a step of removing the resin molded body from a mold.
- a plurality of leads are disposed so as to be separated from each other, and include a first lead and a second lead.
- a liquid thermosetting resin is formed in a space between the first lead and the second lead.
- a resin molded body for a surface-mounted light-emitting device according to any one of 1 to 13, a light-emitting element mounted on the bottom of a recess of the resin molded body and connected to a plurality of leads so as to be energized, and the light-emitting element is sealed
- the surface mount resin molded body of the present invention (hereinafter, simply referred to as “resin molded body” unless otherwise specified) is high because the concave opening surface has a ten-point average roughness in a specific range. It has light reflectivity and is suitable for mass production.
- the resin molded body when the resin molded body is removed from the mold, the resin molded body has good releasability from the mold. Remarkably suppressed. Therefore, according to the present invention, it is possible to mass-produce a resin molded body for a surface-mounted light emitting device having a uniform three-dimensional shape efficiently and at a low defective product rate.
- the present invention by using a cured product having a predetermined glass transition temperature, light reflectance, and light reflectance retention rate as a resin cured body in the resin molded body, good emission luminance can be maintained over a long period of time.
- the resin molding which can be provided can be provided at low cost.
- the resin molded body of the present invention having the technical features 4 to 6 described above is formed in the atmosphere or sealing resin by an Au layer, an Au-based alloy layer, or a bright Ni layer formed as the outermost surface layer in the lead frame thickness direction.
- Chemical degradation due to existing halogen ions, sulfur and the like can be remarkably suppressed.
- maintain further favorable light-emitting luminance over a long term can be provided.
- even if the thickness of the Au layer, the Au-based alloy layer, or the bright Ni layer is very thin, the effect of suppressing chemical deterioration is exhibited, which is advantageous in terms of cost.
- the resin molded body of the present invention having the technical feature 7 described above is designed such that the inner wall surface of the recess of the resin molded body is designed in two steps of a first slope and a second slope with different inclination angles with respect to the bottom surface of the recess.
- the inclination angle By making the inclination angle of 45 ° to 90 ° in particular, it is possible to remarkably suppress the resin chipping at the lead contact portion during mold opening and the occurrence of resin burrs that are likely to occur at the lead portion at the bottom of the recess.
- the manufacturing process can be simplified such as the deburring process can be omitted. Can be provided.
- the inclination angle of the first slope with respect to the bottom surface of the recess is set to 45 ° exceeding 0 ° and the boundary between the first slope and the second slope is a region having a predetermined height from the bottom surface of the recess.
- FIG. It is a top view which shows typically the structure of one Embodiment of the resin molding which concerns on this invention. It is sectional drawing of the resin molding shown in FIG. It is sectional drawing which shows typically the structure of other embodiment of the resin molding which concerns on this invention. It is sectional drawing which shows typically the structure of other embodiment of the resin molding which concerns on this invention. It is a perspective view which shows typically the structure of other embodiment of the resin molding which concerns on this invention. It is sectional drawing which shows typically the structure of other embodiment of the resin molding which concerns on this invention. It is a perspective view which shows typically the structure of the surface mount type light-emitting device containing the resin molding shown in FIG. It is sectional drawing which shows typically the structure of other embodiment of the resin molding which concerns on this invention.
- FIG. 15A is a plan view
- FIG. 15B is a partially enlarged plan view
- FIG. 15C is a partially enlarged sectional view taken along line XX in FIG. 15C.
- the resin molded body of the present invention is formed by integrally molding a resin cured body and a plurality of leads, and has a recess where the plurality of leads are exposed at the bottom, and the ten-point average roughness (hereinafter simply referred to as “Rz”) of the opening surface of the recess.
- Rz ten-point average roughness
- the resin molded body of the present invention is an integrally molded product of a cured resin body having through holes in the thickness direction and a plurality of leads.
- the plurality of leads are fixed to one surface in the thickness direction of the cured resin body by integral molding. Thereby, at least a part of one opening of the through hole of the cured resin body is closed with the plurality of leads, and a recess is formed in the bottom portion where the plurality of leads are exposed.
- the concave portion is opened on the other surface in the thickness direction of the resin molded body. In this specification, this surface is defined as a concave opening surface of the resin molded body.
- the concave opening surface has Rz of 1 ⁇ m to 10 ⁇ m, preferably 1.5 to 7.0 ⁇ m.
- the glass transition temperature of the cured resin body is 10 ° C. or higher
- the light reflectance at 460 nm of the opening surface of the recess is 80% or higher
- the resin molded body is heated at 180 ° C. for 72 hours. It is also characterized in that the retention ratio of the light reflectance of the opening surface of the subsequent recess is 90% or more.
- the glass transition temperature is a value measured using a thermomechanical analyzer (TMA) under conditions of a temperature range of ⁇ 50 to 250 ° C., a heating rate of 5 ° C./min, and a sample size length of 1 to 5 mm.
- TMA thermomechanical analyzer
- the resin molded body of the present invention has these characteristics, and thus has high light reflectance and is suitable for mass production.
- FIG. 1 is a plan view schematically showing a configuration of a resin molded body 1 according to an embodiment of the present invention.
- FIG. 2 is a cross-sectional view of the resin molded body 1 shown in FIG.
- the resin molded body 1 includes a first lead 10 and a second lead 11 as a plurality of leads, and a resin cured body 12, and has a recess 13. Further, in the resin molded body 1, the first lead 10 and the second lead 11 are exposed on at least a part of the outer side surface (side surface in the thickness direction) 1a.
- the resin molded body 1 of the present embodiment has a concave portion 13 having a substantially square planar shape and a thin plate shape, and a substantially circular opening shape at the center thereof. ing.
- the first lead 10 and the second lead 11 are a pair of positive and negative, and are arranged substantially in parallel so as to be separated from each other to form one frame unit (not shown).
- a lead frame is configured by arranging a plurality of frame units in parallel in the vertical and horizontal directions and integrating them.
- the lead frame can be manufactured by punching or etching a thin metal plate.
- the lead frame is formed using a metal material that is a good electrical conductor.
- the metal material is not particularly limited, but a metal material having a volume resistance of less than 0.07 ⁇ ⁇ m and a thermal conductivity of 60 W / (m ⁇ k) or more is preferable.
- iron, phosphor bronze, A copper alloy etc. are mentioned.
- a metal layer such as a plating layer may be formed on at least one of both surfaces of the first lead 10 and the second lead 11 in the thickness direction, particularly on the surface exposed to the bottom 13a of the recess 13. Thereby, the light reflectance of the light emitted from the light emitting element can be further increased.
- the material for the metal layer include gold, silver, copper, and aluminum.
- the thickness is not particularly limited, but is preferably 0.5 ⁇ m to 20 ⁇ m, more preferably 1 ⁇ m to 15 ⁇ m. When the thickness is less than 0.5 ⁇ m, the crystallinity of the metal layer is lowered, and the metal layer is easily discolored due to sulfidation or oxidation.
- the discolored portion absorbs light and easily generates heat, there is a risk of promoting thermal deterioration of the resin molded body 1.
- the metal layer may be easily peeled off from the first and second leads 10 and 11 when the light emitting element is mounted.
- any known method for producing a metal film or a metal thin film can be employed.
- a method for producing a metal film or a metal thin film include electroplating, chemical plating, vapor deposition, sputtering, and diffusion.
- the plating method such as electroplating and chemical plating is preferable in consideration of the denseness of the metal layer to be obtained and the ease of formation.
- a plating layer is preferable.
- the first lead 10 includes a first inner lead portion 10a exposed at the bottom portion 13a of the recess 13 and a first outer lead portion 10b connected to the first inner lead portion 10a and in contact with the cured resin body 12.
- the broken line shown between the 1st inner lead part 10a and the 1st outer lead part 10b has shown these boundaries.
- the second lead 11 includes a second inner lead portion 11 a exposed at the bottom portion 13 a of the concave portion 13 and a second outer lead portion 11 b that is connected to the second inner lead portion 11 a and contacts the cured resin body 12.
- the broken line shown between the 2nd inner lead part 11a and the 1st outer lead part 11b has shown these boundaries.
- an insulating portion 12 b which is a part of a cured resin body 12 described later is interposed to insulate the first and second leads 10 and 11.
- a pair of leads of the first lead 10 and the second lead 11 is used, but the present invention is not limited to this, and an arbitrary number of leads of three or more may be used.
- the cured resin body 12 includes a reflecting portion 12 a that rises outward from the surfaces of the first lead 10 and the second lead 11, and an insulating portion 12 b that is interposed between the first lead 10 and the second lead 11.
- the reflection portion 12a directs light emitted from the light emitting element to the front of the light emitting device when a light emitting device (not shown) is mounted on the surface of the first and second inner lead portions 10a and 11a to produce the light emitting device. And has a function of protecting the light emitting element.
- the top surface of the reflecting portion 12a is the opening surface 12c of the recess 13 in the resin molded body 1 (hereinafter sometimes simply referred to as “opening surface 12c”).
- the insulating portion 12b has a function of supporting the first lead 10 and the second lead 11 and electrically insulating them.
- the opening surface 12c has an Rz of 1 ⁇ m or more and 10 ⁇ m or less.
- the shape of the opening surface 12c is substantially square in the present embodiment, but is not limited to this, and may be, for example, a rectangle, pentagon, hexagon, octagon, ellipse, oval, circle, or the like.
- an oval is a shape which consists of a rectangle and two semicircle which protrudes outward with the diameter of the same length as two sides from two sides which the rectangle opposes.
- the cured resin body 12 has a glass transition temperature of 10 ° C. or higher, preferably 20 ° C. or higher, more preferably 20 ° C. or higher and 250 ° C. or lower, more preferably 30 ° C. or higher and 200 ° C. or lower.
- This glass transition temperature is a value measured using a thermomechanical analyzer (TMA) under the conditions of a temperature range of ⁇ 50 to 250 ° C., a heating rate of 5 ° C./min, and a sample size length of 1 to 5 mm.
- TMA thermomechanical analyzer
- the cured resin body 12 has high heat resistance, and even when it is exposed to a high temperature caused by the light emitting element, thermal deterioration accompanied with discoloration is suppressed. . As a result, the light reflectance at the initial stage of use can be maintained at a high level.
- the opening surface 12c of the cured resin body 12 has a light reflectance at 460 nm of 80% or more, and the retention ratio of the light reflectance on the opening surface 12c after the cured resin body 12 is heated at 180 ° C. for 72 hours. Is 90% or more.
- solid 13 C NMR spectrum at least one peak top in the solid 13 C-nuclear magnetic resonance spectrum (hereinafter referred to as “solid 13 C NMR spectrum”) of the cured resin 12 is present in the range of ⁇ 1 ppm to 2 ppm and 13 ppm to 18 ppm. preferable.
- Such a cured resin body 12 further improves the reliability of the surface-mounted light emitting device.
- the resin material for obtaining the cured resin body 12 having the above characteristics will be described in detail later. Further, the glass transition temperature, light reflectance, retention of light reflectance, and measurement method of solid 13 CNMR spectrum will be described in detail in Examples below.
- the concave portion 13 formed by the first lead 10 and the second lead 11 and the cured resin body 12 includes a bottom portion 13a exposed in a state where the insulating portion 12b is sandwiched between the first lead 10 and the second lead 11, and a resin. It has an inner wall surface 13b which is also an inner slope of the reflecting portion 12a of the cured body 12.
- a light emitting element is mounted on the bottom 13a.
- the inner wall surface 13b is a reflecting surface that reflects light emitted from the light emitting element forward.
- the inclination angle of the inner wall surface 13b of the recess 13 with respect to the bottom 13a is substantially constant. Accordingly, the recess 13 is formed such that the inner diameter thereof continuously increases at a substantially constant rate as the distance from the bottom 13a increases. That is, the concave portion 13 has an inner frustoconical shape, and the inner wall surface 13b is inclined so that it has a wide opening in the opening direction. Thereby, the reflection efficiency of the light emitted from the light emitting element is improved. Moreover, the peelability of the resin molded body 1 from the mold is improved during transfer molding.
- the shape of the internal space of the recess 13 is an inverted truncated cone in this embodiment, but is not limited to this, and may be, for example, a cylindrical shape, a prismatic shape, or the like.
- the inclination angle of the inner wall surface 13b with respect to the bottom surface of the recess 13 is not particularly limited, but is preferably 30 ° to 85 °, more preferably 60 ° to 80 °.
- the bottom surface of the recess 13 means the surface of the bottom 13 a of the recess 13.
- the bottom surface of the recess 13 may be referred to as a horizontal plane of the recess 13.
- the inclination angle of the inner wall surface 13b with respect to the bottom surface of the recess 13 is substantially constant.
- the inner wall surface 13b may be composed of two or more surfaces having different inclination angles. good.
- the inclination angle of at least one surface with respect to the bottom surface of the recess 13 is 70 ° to 80 °.
- the surface near the bottom portion 13a has an inclination angle of 40 ° to 60 ° with respect to the bottom surface of the bottom portion 13a
- the surface near the opening surface 12c has an inclination angle with respect to the bottom surface of the bottom portion 13a of 70 ° to 90 ° is preferred.
- the inner wall surface 13b with respect to the bottom surface of the recess 13 is The inclination angle may be appropriately changed according to a reference different from the above.
- the inclination angle of the inner wall surface 13b with respect to the bottom surface of the recess 13 is set to 70 to 95 °.
- the inclination angle of the inner wall surface 13b with respect to the bottom surface is preferably 55 to 70 °.
- the shape of the bottom 13a of the recess 13 is circular in the present embodiment, but is not limited thereto, and may be, for example, an ellipse, an oval (oval), a square, a rectangle, a hexagon, or an octagon.
- the area of the bottom 13a of the recess 13 is preferably 7 mm 2 or more. By having such an area, for example, a plurality of light emitting elements can be easily mounted.
- the depth of the recess 13 is not particularly limited, but is preferably 0.5 to 5 mm, more preferably 0.5 to 2 mm. On the other hand, the depth of the recess 13 is preferably 450 ⁇ m or less, more preferably 250 to 450 ⁇ m. In this way, by minimizing the depth of the recess 13 and increasing the inclination angle of the inner wall surface 13b with respect to the bottom portion 13a, it is possible to increase the luminous intensity and the amount of light in the side light emitting device.
- the opening shape of the recess 13 in the opening surface 12c is substantially circular in the present embodiment, but is not limited thereto, and may be, for example, elliptical, oval (oval), oval, rectangular, pentagonal, hexagonal, or the like.
- the three-dimensional shape of the resin molded body 1 is substantially flat in the present embodiment, but is not limited thereto, and is appropriately selected from various shapes according to the design of the light emitting device.
- FIG. 3 is a cross-sectional view schematically showing a configuration of a resin molded body 2 according to another embodiment of the present invention.
- members common to the resin molded body 1 are denoted by the same reference numerals as those of the resin molded body 1 and description thereof is omitted.
- the resin molded body 2 has a cured resin body 14 on the opposite side of the cured resin body 12 via the first and second leads 10 and 11, and one end portions of the first and second leads 10 and 11 are outside thereof. It protrudes in the reverse direction from the side surface 2a, respectively.
- the cured resin body 14 has a recess 15 that is recessed on the opposite side of the recess 13 at a position corresponding to the recess 13.
- the cured resin body 14 has substantially the same planar shape and three-dimensional shape as the resin molded body 2 except that its height is lower than that of the cured resin body 2. That is, the three-dimensional shape of the internal space of the recess 15 is an inverted truncated cone in the present embodiment, but is not limited thereto, and may be, for example, a cylindrical shape or a prismatic shape.
- the opening shape of the recess 15 is substantially circular in the present embodiment, but is not limited thereto, and may be, for example, a circular shape, a circular shape, an oval shape, a rectangular shape, a pentagonal shape, or a hexagonal shape.
- the resin material for obtaining the cured resin body 14 may be the same as or different from the resin material for obtaining the cured resin body 2. That is, as the resin material for the cured resin body 14, a resin material described later in this specification can be used, and a conventional resin material used for a resin molded body for a surface-mounted light-emitting device can be used.
- the first and second leads 10 and 11 are less likely to come into direct contact with other components and devices. For example, the first and second leads 10 and 11 are mounted later. The light emitting element is reliably protected.
- FIG. 4 is a cross-sectional view schematically showing a configuration of a resin molded body 3 according to another embodiment of the present invention.
- members common to the resin molded body 1 are denoted by the same reference numerals as those of the resin molded body 1 and description thereof is omitted.
- the resin molded body 3 has a cured resin body 16 on the opposite side of the cured resin body 12 via the first lead 10 and the second lead 11, and one end portions of the first and second leads 10 and 11 are outside thereof. It protrudes from the side surface 3a in the opposite direction.
- the cured resin body 16 has a substantially square planar shape and a flat three-dimensional shape, is in contact with the first and second inner lead portions 10a and 11a and the insulating portion 12b, and further, the first and second outer lead portions. 10b and 11b are in contact with each part.
- the resin material for obtaining the cured resin body 16 the same resin material as that for obtaining the cured resin body 14 can be used.
- the rigidity of the entire resin molded body 3 is increased, and the first and second leads 10, 11 and the insulating layer 12 b are in direct contact with other components and devices (not shown). Is reliably prevented, for example, the first and second leads 10 and 11 and the light emitting element mounted later are more reliably protected.
- FIG. 5 is a perspective view schematically showing a configuration of a resin molded body 4 according to another embodiment of the present invention.
- members common to the resin molded body 1 are denoted by the same reference numerals as those of the resin molded body 1 and description thereof is omitted.
- the resin molded body 4 has a flat three-dimensional shape in which the first and second leads 10 and 11 and the cured resin body 17 are integrally molded, and the first and second outer lead portions 10b and 11b are formed on the outer surface 4a. , 4b, 4c, and 4d, two portions are exposed at each of the four corners.
- the resin molded body 4 has an exposed surface of the cured resin body 17 and an exposed surface of the first and second outer lead portions 10b, 11b on the outer side surfaces 4a, 4b, 4c, 4d substantially on the same plane. It exists in Further, although not shown in FIG. 5, the resin molded body 4 has a metal layer such as a plating layer on the surface of the first lead 10 and / or the second lead 11 in the thickness direction, and the outer surfaces 4a, 4b, 4c. , 4d, the exposed surfaces of the first and second outer lead portions 10b, 11b may be configured not to have a metal layer.
- the material of the metal layer is the same material as the metal layer that the resin molded body 1 may have.
- the first lead 10, the second lead 11, and the resin cured body 17 are integrally formed and have a recess 13.
- the opening surface 17c of the recess 13 has an Rz of 1 ⁇ m or more and 10 ⁇ m or less.
- the insulating layer 17b is exposed on the bottom surface of the recess 13 while being sandwiched between the first inner lead portion 10a and the second inner lead portion 11a.
- the resin molded body 4 is described, for example, in FIG. 1 of JP 2010-62272 A. Also by adopting such a configuration, the first lead 10 and the second lead 11 can be reliably protected, and the reliability of the surface mount light emitting device using the resin molded body 4 can be enhanced.
- a resin molded body according to another embodiment of the present invention is a resin molded body in which a cured resin body and a plurality of leads are integrally formed, and has a recess in which the plurality of leads are exposed at the bottom, wherein the lead electrode
- the lead-shaped surface of the package has a plating layer, and the outermost surface layer is 0.003 to 0.05 ⁇ m Au, and is a ten-point average roughness of the opening surface of the recess.
- Rz is not less than 1 ⁇ m and not more than 10 ⁇ m, and is measured using a thermomechanical analyzer (TMA) in a temperature range of ⁇ 50 to 250 ° C., a heating rate of 5 ° C./min, and a sample size length of 1 to 5 mm.
- TMA thermomechanical analyzer
- the glass transition temperature of the cured resin body was 10 ° C. or higher, the light reflectance at 460 nm of the opening surface of the cured resin body was 80% or higher, and the cured resin body was heated at 180 ° C. for 72 hours. After the opening surface and the The light reflectance retention on the inner wall surface is 90% or more.
- Examples of the resin molded body according to another embodiment include a resin molded body 5 shown in FIGS. 6 and 7.
- FIG. 6 is a cross-sectional view schematically showing a configuration of a resin molded body 5 according to another embodiment of the present invention.
- FIG. 7 is a perspective view schematically showing a configuration of a surface-mounted light emitting device 50 in which the light emitting element 51 is mounted on the resin molded body 5 shown in FIG. 6 and 7, members common to the resin molded body 1 are denoted by the same reference numerals as those of the resin molded body 1 and description thereof is omitted.
- the resin molded body 5 has a plating layer 18 as a metal layer on the surface in the thickness direction of the lead electrodes (first lead 10 and second lead 11) (surface on the side in contact with the cured resin body 12).
- the 18 outermost surface layers 18a are made of Au of 0.003 to 0.05 ⁇ m.
- the resin molded body 5 is a resin except that the first and second leads 10 and 11 have a plating layer 18 on the surface of the first and second inner lead portions 10a and 11a on the surface in contact with the cured resin body 17. It has the same configuration as the molded body 1.
- the cured resin body 17 has the same structure as the cured resin body 17 in the resin molded body 4.
- the plating layer 18 includes an outermost surface layer 18a and a second metal layer 18b interposed between the surface in the thickness direction of the first and second inner lead portions 10a and 11a and the outermost surface layer 18a.
- the plating layer 18 is composed of two plating layers of different materials.
- the outermost surface layer 18a is an Au plating layer having a thickness of 0.003 to 0.05 ⁇ m.
- the first and second inner lead portions 10a and 11a provided with the plating layer 18 are excellent in light reflectivity. Therefore, particularly when the resin molded body 5 is used in a semiconductor light emitting device, The back light can be reflected efficiently and high luminous efficiency can be realized as a whole device.
- the plating layer 18 may be provided not only on the first and second inner lead portions 10a and 11a but also on the first and second outer lead portions 10b and 11b. As a result, the thermal stability of the first and second outer lead portions 10b and 11b and thus the solderability are significantly improved.
- the plating layer 18 is provided on one surface of the first and second inner lead portions 10a and 11a.
- the present invention is not limited to this, and the plating layer 18 may be provided on both surfaces. Further, the plating layer 18 may be provided on the entire surface of both or one of the first and second leads 10 and 11. Further, by forming the outermost surface layer 18a which is an Au plating layer having a thickness of 0.003 to 0.05 ⁇ m, it is possible to achieve both improvement in sulfidation resistance and light reflectance and reduction in material cost.
- the lower limit of the thickness of the Au plating layer that is the outermost surface layer 18a is 0.003 ⁇ m or more, and preferably 0.005 ⁇ m or more, from the viewpoint of sulfidation resistance.
- the upper limit of the thickness of the Au plating layer is 0.05 ⁇ m or less. Yes, 0.03 ⁇ m or less is preferable.
- the outermost surface layer 18a is an Au plating layer in the present embodiment, the outermost layer 18a is not limited thereto, and may be an Au-based alloy plating layer. Examples of the Au-based alloy include an Ag—Au alloy and an Ag—Nd—Au alloy.
- the second metal layer 18b is a plating layer made of a metal such as Au, Ag, Cu, Pd, Ni, or Al.
- a metal such as Au, Ag, Cu, Pd, Ni, Al and the like are preferable, and Ag, Pd, Ni and the like are more preferable from the viewpoint of reducing the cost.
- a Pd plating layer, an Ag plating layer, a laminate of an Ag plating layer and a Pd plating layer, and the like are more preferable.
- Each plating layer constituting the second metal layer 18b exhibits, for example, the following excellent characteristics.
- the silver plating layer not only realizes excellent light reflectance, but also has excellent connectivity with the light emitting element to be mounted and wire bonding.
- the palladium plating layer is chemically stable and has excellent corrosion resistance in a high temperature environment.
- the nickel plating layer has characteristics as a base plating and contributes to wire bonding properties, solderability by lead-free solder, corrosion resistance, and adhesion to the cured resin body 12 forming the envelope.
- the lead frame for semiconductor devices (first and second leads 10 and 11) of the present invention has the plating layer 18 on the surface of the inner part (first and second inner lead parts 10a and 11a).
- the outermost surface layer 18a of the plating layer 18 achieves good light reflectance by a characteristic configuration in which it is a gold or gold-based alloy plating layer.
- the thickness of the plating layer 18 is not particularly limited, and the material of the first and second leads 10 and 11 and the second metal layer 18b, the thickness of the first and second leads 10 and 11, and the resin constituting the cured resin body 12 are not limited. It can be suitably selected according to various conditions such as the type and use of the finally obtained light emitting element.
- the thickness of the plating layer 18 is preferably 0.5 ⁇ m to 20 ⁇ m, and more preferably 1 ⁇ m to 15 ⁇ m.
- the thickness is less than 0.5 ⁇ m, the crystallinity of the plating layer 18 becomes low, and it is easy to be discolored due to sulfidation or oxidation.
- the discolored portion absorbs light and easily generates heat, there is a risk of promoting thermal deterioration of the resin molded body 5.
- the film thickness exceeds 20 ⁇ m, the plating layer 18 is easily peeled off from the first lead 10 or the second lead 11 when the light emitting element is mounted.
- the method for forming the plating layer 18 is not particularly limited, and any known plating method can be adopted. For example, a reel-to-reel method, a dip plating method using a rack, and the like are most preferable. Furthermore, when the plating layer 18 is provided on the surfaces of the first and second inner lead portions 10a and 11a of the first and second leads 10 and 11 as in this embodiment, the plating treatment is performed after the resin molded body 5 is formed. May be. Such a plating process is called a post-plating process.
- the plating layer 18 is provided as a metal layer on the surfaces of the first and second inner lead portions 10a and 11a of the first and second leads 10 and 11, but is not limited to the plating layer and other than the plating layer.
- Various metal layers can be formed.
- any known method for forming a metal layer can be employed, and examples thereof include electroplating, chemical plating, vapor deposition, sputtering, and diffusion.
- FIG. 7 shows a usage example of the resin molded body 5.
- 7 includes a resin molded body 5 having a plating layer 18 on the surfaces of first and second inner lead portions (not shown), and a light emitting element 51 mounted on the first inner lead portion. And a first gold wire 52a that electrically connects the light emitting element 51 and the first inner lead part, and a second gold wire 52b that electrically connects the light emitting element 51 and the second inner lead part.
- the resin molded body 5 has two plating layers made of different materials on the surfaces of the first and second leads, so that thermal deterioration of the first and second leads is particularly suppressed. The reflectivity can be maintained at a high level in the long term, and the long term reliability is very high.
- a resin molded body according to another embodiment of the present invention is a resin molded body in which a cured resin body and a plurality of leads are integrally molded, and has a recess in which the plurality of leads are exposed at the bottom,
- the first resin molded body slope contacting the lead has an angle from the lead horizontal plane of 45 ° or less
- the second resin molded body slope generated from a height of 100 ⁇ m or less from the lead horizontal plane is relative to the lead horizontal plane.
- 45 ° to 90 ° the bottom surface of the recess opening is the surface of the lead exposed at the bottom of the recess, and is also the horizontal surface of the lead.
- the inner wall surface of the recess is composed of two slopes having different inclination angles with respect to the lead horizontal plane, that is, a first resin molded body slope and a second resin molded body slope.
- the inclination angle with respect to the lead horizontal plane is an angle formed by the lead horizontal plane and the first or second resin molded body slope in the cross-sectional view in the thickness direction of the resin molded body for the surface-mounted light-emitting device.
- the resin molded body of such an embodiment when a light emitting element is mounted on the molded body, a light reflecting portion that reflects lateral light emitted from the light emitting element in the front direction (perpendicular to the bottom of the recess) and
- the lead contact portion of the inner resin molding portion (the inner wall surface of the concave portion) is designed to be stepped in a range from an acute angle to a vertical angle than the slope angle of the resin molding portion. More specifically, in the resin molded body in which the cured resin body and the plurality of leads are integrally formed and the bottom portion has a recess in which the plurality of leads are exposed, the resin molded body first contacting the lead on the bottom surface of the recess opening. When the slope is 45 ° or less from the lead horizontal plane, the second slope of the resin molded body is 45 ° to 90 ° with respect to the lead horizontal plane so that a height of 100 ⁇ m or less is generated from the lead horizontal plane. Like that.
- FIG. 8 is a cross-sectional view schematically showing a configuration of a resin molded body 6 according to another embodiment of the present invention.
- FIG. 9 is a cross-sectional view schematically showing the occurrence of a resin burr 58 and a resin chip 59 in a conventional resin molded body 55.
- members common to the resin molded body 1 are denoted by the same reference numerals as those of the resin molded body 1 and description thereof is omitted.
- the first and second leads 10 and 11 and the cured resin body 19 are integrally formed, and the inner wall surface 13 b of the recess 13 is constituted by the first inclined surface 61 and the second inclined surface 60, and the step is formed.
- the other structure is the same as that of the resin molded body 1.
- the second inclined surface 60 rises from the periphery of the bottom surface continuously to the bottom surface of the recess 13 and has an inclination angle ⁇ 2 with respect to the bottom surface in the range of 45 ° to 90 °.
- the bottom surface of the concave portion 13 is the surface of the first and second leads 10 and 11 (that is, the first and second inner lead portions 10a and 11a) exposed at the bottom portion 13a of the concave portion 13.
- the bottom surface of the recess 13 is also called a lead horizontal plane.
- the inclination angle ⁇ 2 with respect to the bottom surface of the second slope 60 is an angle formed by the bottom surface of the recess 13 and the second slope 60 in FIG.
- the first inclined surface 61 rises from the periphery of the second inclined surface 60 toward the opening surface 19c continuously to the second inclined surface 60, and the inclination angle ⁇ 1 with respect to the bottom surface is more than 0 ° and not more than 45 °.
- the inclination angle ⁇ ⁇ b> 1 with respect to the bottom surface of the first slope 61 is an angle formed by the bottom surface of the recess 13 and a virtual line extending linearly from the first slope 61 toward the bottom surface.
- the boundary between the second inclined surface 60 and the first inclined surface 61 is at a position where the height (h in FIG. 8) exceeds 0 ⁇ m and is not more than 100 ⁇ m from the bottom surface of the inner wall surface 13b of the recess 13.
- the height (h) from the bottom surface of the recess 13 is in the region of 100 ⁇ m or less between the second inclined surface 60 and the first inclined surface 61 having different inclination angles.
- the first inclined surface 61 and the second inclined surface 60 each having a predetermined inclination angle are provided, the boundary between the first inclined surface 61 and the second inclined surface 60 is provided in a predetermined region, and the inner wall surface of the recess 13 is provided.
- the following effects (a) to (c) can be obtained.
- the height (h) from the bottom surface of the recess 13 at the boundary between the second inclined surface 60 and the first inclined surface 61 is preferably 10 ⁇ m to 100 ⁇ m, more preferably 30 ⁇ m to 80 ⁇ m.
- the reflection efficiency of light emitted from the light emitting element in a direction substantially perpendicular to the bottom surface of the recess 13 is improved. This can improve the commercialization rate of the light emitting device.
- the inclination angle ⁇ 1 of the first inclined surface 61 is preferably 20 ° to 45 °, and more preferably 30 ° to 40 °.
- the resin molded body of the present invention can have various forms as long as Rz of the concave opening surface is 1 ⁇ m or more and 10 ⁇ m or less.
- Rz of the concave opening surface is 1 ⁇ m or more and 10 ⁇ m or less.
- FIGS. 6, 9, and 11 to 13 described in Japanese Patent Application Laid-Open No. 2010-62272 a cured resin, a first lead, and a second lead are integrally formed, and a resin having a flat three-dimensional shape.
- a shaped body is shown.
- the resin molded body has a recess having a circular opening shape, and the bottom of the recess is exposed in a state where the first lead and the second lead are opposed to each other through an insulating portion, and the shape of the opening surface of the recess is rectangular. It is.
- the resin cured body and the first lead or the second lead are formed at the four corners of the resin molded body. There is a step at the boundary.
- the resin cured body has a missing portion extending from one side surface in the lateral direction to the other side surface at the lower part of the two side surfaces facing in the vertical direction.
- the vertical cross-sectional shape is T-shaped. A part of the first lead and the second lead are exposed at two missing portions of the cured resin body, respectively.
- the exposed portion of the first lead extends from one side surface in the horizontal direction to the other side surface, and the vertical cross section has a shape in which the L-shape is rotated 90 ° to the right.
- the exposed portion of the second lead extends from one side surface in the horizontal direction to the other side surface, and the vertical cross section has a shape in which the L-shape is rotated 90 ° to the right and then reversed left and right. .
- the exposed surface of the cured resin body and the exposed surfaces of the first lead and the second lead are substantially on the same plane.
- the cured resin body has a missing portion extending from one side surface in the lateral direction to the other side surface at the lower part of the two side surfaces facing in the vertical direction.
- the vertical cross-sectional shape is T-shaped. A part of the first lead and the second lead are exposed at two missing portions of the cured resin body, respectively.
- the exposed portions of the first lead and the second lead respectively extend from one side surface in the horizontal direction to the other side surface, and the vertical cross-sectional shape is rectangular. Furthermore, in the substantially central portion in the horizontal direction in these exposed portions, the vertical cross-sectional shape is rectangular, and has a missing portion extending in the horizontal direction.
- a plating layer may be formed on each surface facing the missing portion. Furthermore, a plating layer may be formed on at least a part of the first lead and the second lead exposed at the bottom of the resin molded body.
- the first lead and the second lead are exposed at the bottom of the four corners of the side surface in the thickness direction and at the bottom of the two side surfaces facing in the vertical direction. is doing.
- the first lead is exposed at the bottom of two corners adjacent in the horizontal direction among the four corners and at the bottom of one side surface facing in the vertical direction.
- a cured resin is interposed between the first lead exposed at the two corners and the first lead exposed at the side surface.
- the first lead exposed on the side surface extends in the lateral direction, and has a missing portion (a rectangular parallelepiped space) extending in the lateral direction, similar to the resin molded body shown in FIG. 11 of Japanese Patent Application Laid-Open No. 2010-62272. .
- a plating layer may be formed on each surface facing the missing portion.
- the second lead is exposed at the bottom of two corners adjacent in the lateral direction other than the two corners where the first lead is exposed, and at the bottom of the other side opposite to the vertical direction. It has the same configuration as the exposed portion.
- a plating layer may be formed on at least a part of the first lead and the second lead exposed at the bottom of the resin molded body.
- the resin cured body has a missing portion extending from one side surface in the lateral direction to the other side surface at the lower part of the two side surfaces facing in the vertical direction.
- the vertical cross-sectional shape is T-shaped.
- the space shape of the missing part is substantially a rectangular parallelepiped. A part of the first lead and the second lead are exposed at two missing portions of the cured resin body, respectively.
- the first lead is exposed at a lower portion of one side surface in the vertical direction, extends from one side surface in the horizontal direction to the other side surface, has a rectangular cross-sectional shape in a substantially central portion in the horizontal direction, and extends in the horizontal direction. There are missing parts in two adjacent corners.
- the space shape of the missing portion is a rectangular parallelepiped shape or a cubic shape.
- the second lead has the same configuration as the first lead except that it is exposed at the lower portion of the other side surface in the vertical direction.
- the resin material for obtaining the resin cured body for reflecting the light emitted from the light emitting element is not particularly limited, but from the viewpoint of carrying out transfer molding, a thermosetting resin is used. It is preferable to use it.
- a thermosetting resin those used in the field of surface-mounted light-emitting devices can be used without particular limitation, and examples thereof include epoxy resins, modified epoxy resins, silicone resins, modified silicone resins, acrylate resins, and polyurethanes. It is done. These thermosetting resins can be used alone or in combination of two or more.
- thermosetting resins epoxy resins, modified epoxy resins, silicone resins and modified silicone resins are preferable.
- 100 parts by weight of a mixture of an epoxy resin and an equivalent acid anhydride, 0.1 to 2 parts by weight of a curing accelerator, 0.5 to 3 parts by weight of a promoter, 5 to 30 parts by weight of a white pigment and 30 inorganic fillers An epoxy resin composition obtained by adding ⁇ 70 parts by weight can be used.
- an epoxy resin composition that has been partially cured by heating to a B-stage can be used.
- examples of the epoxy resin include an epoxy resin obtained from triglycidyl isocyanurate, hydrogenated bisphenol A diglycidyl ether, and the like.
- examples of the acid anhydride include hexahydrophthalic anhydride, 3-methylhexahydrophthalic anhydride, 4-methylhexahydrophthalic anhydride, and the like.
- examples of the curing accelerator include DBU (1,8-diazabicyclo [5,4,0] undecene-7).
- examples of the cocatalyst include ethylene glycol.
- examples of the white pigment include titanium oxide.
- examples of the inorganic filler include silica particles and glass fibers.
- thermosetting resin composition (X) contained is more preferable.
- thermosetting resin composition (X) Since the thermosetting resin composition (X) has a relatively low linear expansion coefficient, the difference from the linear expansion coefficient of the metal material used for the lead is reduced. Moreover, since the thermosetting resin composition (X) has high heat resistance and is unlikely to undergo thermal deterioration with discoloration, the light reflectance is maintained at a high level in the initial stage of use even when exposed to high temperatures.
- the components (A) to (E) will be described in detail below.
- the component (A) is not particularly limited as long as it is an organic compound containing at least two carbon-carbon double bonds reactive with SiH groups in one molecule.
- the skeleton of the component (A) does not contain a siloxane unit (Si—O—Si) as an organic compound, such as polysiloxane-organic block copolymer or polysiloxane-organic graft copolymer. More preferred are compounds containing no elements other than N, O, S and halogen. In the case of those containing siloxane units, there is a problem that the adhesiveness between the semiconductor package and the lead frame or the sealing resin tends to be low.
- the component (A) can be classified into an organic polymer compound and an organic monomer compound.
- Examples of the component (A) that is an organic polymer compound include polyether, polyester, polyarylate, polycarbonate, saturated hydrocarbon, unsaturated hydrocarbon, polyacrylate ester, polyamide, and phenol. Examples thereof include those having a formaldehyde-based (phenolic resin-based) or polyimide-based skeleton.
- examples of the polyether polymer include polyoxyethylene, polyoxypropylene, polyoxytetramethylene, polyoxyethylene-polyoxypropylene copolymer, and the like. More specific examples include polymers represented by the following [Chemical Formula 1].
- R 1 and R 2 are C, H, N, O, S, C 1 -C 6 divalent organic groups not containing any elements other than halogen as constituent elements, n, m, and l are 1 to Represents a number of 300.
- organic polymer compounds examples include dibasic acids such as adipic acid, phthalic acid, isophthalic acid, terephthalic acid and hexahydrophthalic acid, and ethylene glycol, diethylene glycol, propylene glycol, tetramethylene glycol, neopentyl glycol and the like.
- Polyester polymers obtained by condensation with glycols or ring-opening polymerization of lactones; ethylene-propylene copolymers, polyisobutylene, copolymers of isobutylene and isoprene, polychloroprene, polyisoprene, isoprene and butadiene, Copolymers of acrylonitrile, styrene, etc., polybutadiene, copolymers of butadiene and styrene, acrylonitrile, etc., polyisoprene, polybutadiene, isoprene or butadiene and acrylonitrile
- Polyolefin-based (saturated hydrocarbon-based) polymer obtained by hydrogenating a copolymer with styrene, styrene, etc .
- polyacrylate ester ethyl acrylate, obtained by radical polymerization of monomers such as ethyl acrylate, butyl
- an alkenyl group having a carbon-carbon double bond can be introduced into the polymer skeleton of the organic polymer compound to obtain the component (A).
- the alkenyl group having a carbon-carbon double bond may be present anywhere in the molecule, but is preferably present in the side chain or terminal of the polymer skeleton from the viewpoint of reactivity.
- an organic polymer having a functional group such as a hydroxyl group, an alkoxide group, a carboxyl group or an epoxy group at the terminal, main chain or side chain is reactive with the functional group.
- an organic compound having both an active group having an alkenyl group and an alkenyl group an alkenyl group can be introduced into the terminal, main chain or side chain.
- Examples of the organic compound having both an active group and an alkenyl group reactive to the functional group include 3 to 20 carbon atoms such as acrylic acid, methacrylic acid, vinyl acetic acid, acrylic acid chloride, and acrylic acid bromide.
- This method is a method of transesterifying an alcohol residue of an ester portion of a polyester resin or an acrylic resin with an alkenyl group-containing alcohol or an alkenyl group-containing phenol derivative using a transesterification catalyst.
- the alkenyl group-containing alcohol and alkenyl group-containing phenol derivative used for transesterification with an alcohol residue may be any alcohol or phenol derivative having at least one alkenyl group and having at least one hydroxyl group. It is preferable to have one.
- a catalyst may or may not be used, but a titanium-based catalyst and a tin-based catalyst are preferable.
- alkenyl group-containing alcohol examples include vinyl alcohol, allyl alcohol, 3-buten-1-ol, 4-penten-1-ol, 5-hexen-1-ol, 6-hepten-1-ol, and 7-octene. -1-ol, 8-nonen-1-ol, 9-decene-1-ol, 2- (allyloxy) ethanol, neopentyl glycol monoallyl ether, glyceryl diallyl ether, trimethylolpropane triallyl ether, trimethylolethanetri Examples include allyl ether, pentaerythritol tetraallyl ether, 1,2,6-hexanetriol triallyl ether, sorbitan triallyl ether, and the like.
- alkenyl group-containing phenol derivative examples include the compounds shown in the following [Chemical Formula 2].
- allyl alcohol vinyl alcohol, 3-buten-1-ol, 2- (allyloxy) ethanol, and each compound represented by the following [Chemical Formula 3] are preferable from the viewpoint of availability.
- ester residue of the above-mentioned alcohol or phenol derivative such as acetate ester and the ester portion of the polyester resin or acrylic resin are transesterified using a transesterification catalyst, and the alcohol residue in the ester portion of the polyester resin or acrylic resin to be produced is obtained.
- a method of introducing an alkenyl group by a method in which a low molecular weight esterified product such as an acetate of a group is distilled out of the system by vacuum devolatilization or the like.
- an alkenyl group can be introduced at the terminal by a method of terminating the polymerization reaction by bonding a compound having an alkenyl group at the living terminal.
- Examples of a method for introducing an alkenyl group during polymerization include a radical chain transfer agent having an alkenyl group having low radical reactivity when the organic polymer skeleton of the component (A) used in the present invention is produced by radical polymerization. Can be used to introduce an alkenyl group into the side chain or terminal of the organic polymer skeleton.
- Examples of such radical chain transfer agents include vinyl monomers having alkenyl groups with low radical reactivity in the molecule, such as allyl methacrylate and allyl acrylate, and allyl mercaptans.
- the molecular weight of the component (A) is not particularly limited, but any of 100 to 100,000, preferably 300 to 100,000 can be suitably used, and an alkenyl group-containing organic polymer has a molecular weight of 500 to 20,000. Those are particularly preferred. When the molecular weight is less than 300, characteristics due to the use of an organic polymer such as imparting flexibility are hardly exhibited, and when the molecular weight exceeds 100,000, the effect of crosslinking due to the reaction between the alkenyl group and the SiH group is hardly exhibited. .
- component (A) that is an organic monomer compound examples include aromatic hydrocarbons such as phenols, bisphenols, benzene, and naphthalene: aliphatic hydrocarbons such as linear and alicyclic: heterocyclic And compounds of the system and mixtures thereof.
- the bonding position of the carbon-carbon double bond having reactivity to the SiH group is not particularly limited, and may be present anywhere in the molecule.
- the carbon-carbon double bond having reactivity with respect to the SiH group is not particularly limited, but the general formula (I): CH 2 ⁇ C (R 1 ) — (wherein R 1 is a hydrogen atom or a methyl group) Is preferable from the viewpoint of reactivity.
- R 1 is a hydrogen atom or a methyl group
- a group represented by the formula: CH 2 ⁇ CH— is particularly preferable.
- the carbon-carbon double bond having reactivity with the SiH group of component (A) is represented by the general formula (II): —C (R 2 ) ⁇ C (R 2 ) — (wherein R 2 is a hydrogen atom or methyl).
- R 2 is a hydrogen atom or methyl
- the alicyclic group represented by is preferable from the viewpoint that the cured resin has high heat resistance. In view of the availability of raw materials, an alicyclic group represented by the formula: —CH ⁇ CH— is particularly preferred.
- the carbon-carbon double bond having reactivity to the SiH group may be directly bonded to the skeleton of the component (A) or may be covalently bonded via a divalent or higher substituent.
- the divalent or higher valent substituent is not particularly limited as long as it is a substituent having 0 to 10 carbon atoms. However, a constituent element containing no element other than C, H, N, O, S and halogen is preferable. Examples of these substituents include compounds represented by the following [Chemical 4] and [Chemical 5]. Moreover, two or more of these divalent or higher valent substituents may be connected by a covalent bond to constitute one divalent or higher valent substituent.
- Examples of the group covalently bonded to the skeleton as described above include vinyl group, allyl group, methallyl group, acrylic group, methacryl group, 2-hydroxy-3- (allyloxy) propyl group, 2-allylphenyl group, 3 -Allylphenyl group, 4-allylphenyl group, 2- (allyloxy) phenyl group, 3- (allyloxy) phenyl group, 4- (allyloxy) phenyl group, 2- (allyloxy) ethyl group, 2,2-bis (allyl) Examples thereof include an oxymethyl) butyl group, a 3-allyloxy-2,2-bis (allyloxymethyl) propyl group, and groups represented by the following [Chemical Formula 6].
- component (A) which is an organic polymer compound examples include 1,2-polybutadiene (1,2 ratio 10 to 100%, preferably 1,2 ratio 50 to 100%), novolak phenol Examples include allyl ether, allylated polyphenylene oxide, and polymers represented by the following [Chemical Formula 7] to [Chemical Formula 11].
- R 1 is H or CH 3
- R 2 , R 3 is a divalent organic group having 1 to 6 carbon atoms that does not contain elements other than C, H, N, O, S, and halogen as constituent elements
- X and Y are divalent substituents having 0 to 10 carbon atoms
- n, m, and l are numbers 1 to 300.
- R 1 is H or CH 3
- R 4 , R 5 is a divalent organic group having 1 to 6 carbon atoms
- X and Y are divalent substituents having 0 to 10 carbon atoms
- n, m, l represents a number from 1 to 300.
- R 1 is H or CH 3
- R 6 , R 7 is a divalent organic group having 1 to 20 carbon atoms
- X and Y are divalent substituents having 0 to 10 carbon atoms
- n, m, l represents a number from 1 to 300.
- R 1 is H or CH 3
- R 8 and R 9 are divalent organic groups having 1 to 6 carbon atoms
- X and Y are divalent substituents having 0 to 10 carbon atoms
- n, m, l represents a number from 1 to 300.
- R 1 is H or CH 3
- R 10 , R 11 , R 12 are divalent organic groups having 1 to 6 carbon atoms
- X and Y are divalent substituents having 0 to 10 carbon atoms
- n , M, l, and p represent a number of 1 to 300).
- component (A) which is an organic monomer compound examples include diallyl phthalate, triallyl trimellitate, diethylene glycol bisallyl carbonate, trimethylolpropane diallyl ether, pentaerythritol triallyl ether, 1,1,2 , 2-tetraallyloxyethane, diarylidenepentaerythritol, triallyl cyanurate, triallyl isocyanurate, 1,2,4-trivinylcyclohexane, divinylbenzenes (having a purity of 50 to 100%, preferably purity 80-100%), divinylbiphenyl, 1,3-diisopropenylbenzene, 1,4-diisopropenylbenzene, and oligomers thereof, as shown in the following [Chemical Formula 12] to [Chemical Formula 13], Conventionally known epoxy resin glycidyl It includes compounds in which a part or all is replaced with an allyl group.
- the component (A) it is also possible to use a low molecular weight compound that is difficult to express by dividing into a skeleton portion and an alkenyl group as described above.
- these low molecular weight compounds include aliphatic chain polyene compound systems such as butadiene, isoprene, octadiene and decadiene, fats such as cyclopentadiene, cyclohexadiene, cyclooctadiene, dicyclopentadiene, tricyclopentadiene and norbornadiene.
- examples thereof include aromatic cyclic polyene compound systems and substituted aliphatic cyclic olefin compound systems such as vinylcyclopentene and vinylcyclohexene.
- a component containing 0.001 mol or more of carbon-carbon double bond having reactivity to the SiH group per 1 g of the component (A) Preferably, what contains 0.005 mol or more per 1 g of component (A), more preferably 0.008 mol or more per 1 g of component (A).
- the average number of carbon-carbon double bonds having reactivity with the SiH group may be at least two per molecule. However, when the mechanical strength is to be further improved, the number is 2. It is preferable that the number exceeds 3, and more preferably 3 or more. When the number of carbon-carbon double bonds reactive to the SiH group of component (A) is 1 or less per molecule, even if component (A) and component (B) react, Only the graft structure is generated, and the crosslinked structure is not generated.
- the component (A) from the viewpoint of good reactivity, it is preferable that one or more vinyl groups are contained in one molecule, and two or more vinyl groups are contained in one molecule. It is more preferable. Further, from the viewpoint that the storage stability tends to be good, it is preferable that 6 or less vinyl groups are contained in one molecule, and it is more preferable that 4 or less vinyl groups are contained in one molecule.
- the molecular weight of the component (A) is such that the mechanical heat resistance is high, the stringiness of the raw material liquid is small, the moldability and the handleability are good, and the powders such as the components (E) and (F) From the standpoint of easy uniform mixing with and a good moldability when making a thermosetting resin composition tablet, it is preferably less than 900, more preferably less than 700, and even more preferably less than 500. is there.
- the viscosity of component (A) is preferably less than 1000 poise, more preferably less than 300 poise, and even more preferably 30 poise at 23 ° C. in order to obtain uniform mixing with other components and good workability. Is less than.
- the viscosity can be measured with an E-type viscometer.
- the component (A) preferably has a low content of a compound having a phenolic hydroxyl group and / or a derivative of a phenolic hydroxyl group from the viewpoint of higher light resistance, and is a phenolic hydroxyl group and / or a derivative of a phenolic hydroxyl group. What does not contain the compound which has is preferable.
- the phenolic hydroxyl group in the present invention is a hydroxyl group directly bonded to an aromatic hydrocarbon nucleus exemplified by a benzene ring, naphthalene ring, anthracene ring and the like, and the derivative of the phenolic hydroxyl group is a hydrogen atom of the above-mentioned phenolic hydroxyl group.
- the weight ratio of the aromatic ring component (A) is preferably 50% by weight or less, more preferably 40% by weight or less, and more preferably 30% by weight or less. Are more preferred. Most preferred are those that do not contain an aromatic hydrocarbon ring.
- the component (A) includes vinylcyclohexene, dicyclopentadiene, vinylnorbornene, triallyl isocyanurate, 2,2-bis (4-hydroxycyclohexyl).
- ком ⁇ онент (A) a compound represented by the following general formula (III) is preferable from the viewpoint of particularly high heat resistance and light resistance.
- R 1 in the general formula (III) is preferably a monovalent organic group having 1 to 20 carbon atoms, and more preferably a carbon number, from the viewpoint that the cured resin obtained can have higher heat resistance.
- R 1 examples of these preferable R 1 are methyl group, ethyl group, propyl group, butyl group, phenyl group, benzyl group, phenethyl group, vinyl group, allyl group, glycidyl group, and each of those exemplified below in [Chemical Formula 15]. And monovalent groups.
- R 1 of the general formula (III) the adhesion between the resin molded body and the lead or the resin molded body and the sealing agent can be improved, or the mechanical strength of the obtained resin molded body can be increased.
- at least one of the three R 1 is a monovalent organic group having 1 to 50 carbon atoms including one or more epoxy groups, and the epoxy group represented by the following [Chemical Formula 16] is represented by 1 More preferably, it is a monovalent organic group containing 1 to 50 carbon atoms.
- R 1 examples include a glycidyl group and groups represented by [Chemical Formula 17].
- R 1 in the above general formula (III) is preferably C, H, or O only as a constituent element containing 2 or less oxygen atoms from the viewpoint that the heat resistance of the resulting cured resin can be improved.
- a monovalent organic group having 1 to 50 carbon atoms more preferably a monovalent hydrocarbon group having 1 to 50 carbon atoms.
- these preferable R 1 groups include a methyl group, an ethyl group, a propyl group, a butyl group, a phenyl group, a benzyl group, a phenethyl group, a vinyl group, an allyl group, a glycidyl group, and groups represented by the following [Chemical Formula 18].
- At least one of the three R 1 is a group represented by the formula: —C ( ⁇ CH 2 ) —. It is preferably a monovalent organic group having 1 to 50 carbon atoms and containing at least one.
- at least one of the three R 1 groups is represented by the general formula (IV): CH 2 ⁇ C (R 2 ) — [wherein R 2 represents a hydrogen atom or a methyl group.
- R 3 in the general formula (V) is a direct bond or a divalent organic group having 1 to 48 carbon atoms. From the viewpoint of further improving the heat resistance of the resulting molded resin, it is preferably a direct bond. Or a divalent organic group having 1 to 20 carbon atoms, more preferably a direct bond or a divalent organic group having 1 to 10 carbon atoms, and still more preferably a direct bond or a divalent organic group having 1 to 4 carbon atoms. Organic group. Examples of these preferable R 3 include the groups shown in the following [Chemical Formula 19].
- R 3 in the general formula (V) from the viewpoint of further improving the heat resistance of the obtained resin molding, it is preferably bonded directly or contains two or less oxygen atoms as a constituent element.
- R 4 in the general formula (V) is a hydrogen atom or a methyl group, and a hydrogen atom is preferable from the viewpoint of good reactivity.
- a hydrogen atom is preferable from the viewpoint of good reactivity.
- one molecule contains at least two carbon-carbon double bonds having reactivity to the SiH group. is necessary. From the viewpoint of further improving the heat resistance, it is more preferable to use an organic compound containing three or more carbon-carbon double bonds having reactivity to the SiH group in one molecule.
- organic compound represented by the general formula (III) as described above include triallyl isocyanurate, each compound represented by the following [Chemical Formula 21], and the like.
- an organic material containing at least two carbon-carbon double bonds reactive with SiH groups in one molecule examples include a reaction product of one or more compounds selected from compounds and a compound ( ⁇ ) having a SiH group (hereinafter referred to as “( ⁇ ) component”).
- a reactant has good compatibility with the component (B) and has a low volatility, and therefore has an advantage that the problem of outgas from the obtained resin molded product hardly occurs.
- the ( ⁇ ) component is a compound having a SiH group, and a linear and / or cyclic polyorganosiloxane having a SiH group is also an example.
- a linear and / or cyclic polyorganosiloxane having a SiH group is also an example.
- compounds represented by [Chemical Formula 22] to [Chemical Formula 23] are exemplified.
- a cyclic polyorganosiloxane having at least 3 SiH groups per molecule is preferred.
- R 1 represents an organic group having 1 to 6 carbon atoms, and n represents a number of 3 to 10).
- the substituent R 1 in the compound represented by the general formula (VI) is preferably a group that does not contain a constituent element other than C, H, and O, more preferably a hydrocarbon group, and still more preferably a methyl group. It is. In view of availability, the compound represented by the general formula (VI) is preferably 1,3,5,7-tetramethylcyclotetrasiloxane.
- ( ⁇ ) component examples include compounds having a SiH group such as bisdimethylsilylbenzene.
- Various ( ⁇ ) components as described above can be used singly or in combination of two or more.
- the present invention as described above, it is obtained by hydrosilylation reaction of an organic compound containing at least two carbon-carbon double bonds having a reactivity to SiH group in one molecule and the ( ⁇ ) component.
- the compound obtained can be used as the component (A).
- the component (A) of the present invention is obtained.
- a mixture containing the obtained compound and a plurality of other compounds may be obtained.
- the thermosetting resin composition of the present invention can also be produced by using as it is without separating the compound that can be the component (A) from such a mixture.
- the mixing ratio of the organic compound containing at least two carbon-carbon double bonds having reactivity to SiH group in one molecule and the ( ⁇ ) component is not particularly limited.
- the ratio between the total number of carbon-carbon double bonds (X) having reactivity with SiH groups in the former and the total number of SiH groups (Y) in the latter is reduced.
- the compatibility of the component (A) with the component (B) is easily improved, preferably 10 ⁇ X / Y, more preferably 5 ⁇ X / Y.
- catalysts other than platinum compounds include RhCl (PPh) 3 , RhCl 3 , RhAl 2 O 3 , RuCl 3 , IrCl 3 , FeCl 3 , AlCl 3 , PdCl 2 .2H 2 O, NiCl 2 , TiCl 4. Etc.
- chloroplatinic acid, platinum-olefin complexes, platinum-vinylsiloxane complexes and the like are preferable from the viewpoint of catalytic activity.
- these catalysts can be used individually by 1 type or in combination of 2 or more types.
- the addition amount of the catalyst is not particularly limited, but in order to obtain a thermosetting resin composition having sufficient curability and a relatively low cost, it can be used with respect to 1 mole of SiH group of the ( ⁇ ) component. , Preferably 10 ⁇ 8 to 10 ⁇ 1 mol, more preferably 10 ⁇ 6 to 10 ⁇ 2 mol.
- a co-catalyst can be used with the said catalyst.
- the cocatalyst include phosphorus compounds such as triphenylphosphine, 1,2-diester compounds such as dimethyl malate, acetylene alcohol compounds such as 2-hydroxy-2-methyl-1-butyne, Examples thereof include sulfur compounds such as sulfur and amine compounds such as triethylamine.
- the amount of the cocatalyst added is not particularly limited, but is preferably 10 ⁇ 2 to 10 2 mol, more preferably 10 ⁇ 1 mol to 10 mol, per 1 mol of the hydrosilylation catalyst.
- various methods can be used as a method of mixing an organic compound containing at least two carbon-carbon double bonds that are reactive to SiH groups in one molecule, the component ( ⁇ ), and a catalyst.
- the catalyst can be mixed with an organic compound containing at least two carbon-carbon double bonds that are reactive to SiH groups in one molecule, and the resulting mixture is mixed with the ( ⁇ ) component. Is preferred.
- reaction It may be difficult to control.
- the reaction temperature can be variously set, but is preferably 30 ° C to 200 ° C, more preferably 50 ° C to 150 ° C. If the reaction temperature is low, the reaction time for sufficient reaction will be long, and if the reaction temperature is high, it is not practical.
- the reaction may be carried out at a constant temperature, but the temperature may be changed in multiple steps or continuously as required. Various reaction times and pressures during the reaction can be set as required.
- a solvent may be used for the hydrosilylation reaction.
- Solvents that can be used are not particularly limited as long as they do not inhibit the hydrosilylation reaction. Specific examples include hydrocarbon solvents such as benzene, toluene, hexane, heptane, tetrahydrofuran, 1,4-dioxane, 1, Ether solvents such as 3-dioxolane and diethyl ether, ketone solvents such as acetone and methyl ethyl ketone, and halogen solvents such as chloroform, methylene chloride and 1,2-dichloroethane can be preferably used.
- the solvent can also be used as a mixed solvent of two or more types.
- solvents toluene, tetrahydrofuran, 1,3-dioxolane and chloroform are preferable.
- the amount of solvent to be used can also be set as appropriate.
- various additives may be used for the purpose of controlling reactivity.
- the upper limit of the temperature in this case is preferably 100 ° C, more preferably 60 ° C.
- the component (A) is a hydrosilylation reaction product of an organic compound containing at least two carbon-carbon double bonds having a reactivity with respect to the SiH group in one molecule and the component ( ⁇ ).
- Examples include a reaction product of bisphenol A diallyl ether and 1,3,5,7-tetramethylcyclotetrasiloxane, a reaction product of vinylcyclohexene and 1,3,5,7-tetramethylcyclotetrasiloxane, divinylbenzene and 1 , 3,5,7-tetramethylcyclotetrasiloxane reactant, dicyclopentadiene and 1,3,5,7-tetramethylcyclotetrasiloxane reactant, triallyl isocyanurate and 1,3,5,7- Reactant of tetramethylcyclotetrasiloxane, diallyl monoglycidyl isocyanurate and 1,3,5,7-tetramethyl
- the component (A) may have other reactive groups.
- the reactive group in this case include an epoxy group, an amino group, a radical polymerizable unsaturated group, a carboxyl group, an isocyanate group, a hydroxyl group, and an alkoxysilyl group.
- an epoxy group is preferable from the viewpoint that the adhesiveness can be further increased.
- a component can be used individually by 1 type or in combination of 2 or more types.
- the component (B) is a compound containing at least two SiH groups in one molecule.
- the component (B) is not particularly limited as long as it is a compound containing at least two SiH groups in one molecule.
- the compound described in International Publication WO96 / 15194 is at least two in one molecule. Those having SiH groups can be used.
- a chain and / or cyclic organopolysiloxane having at least two SiH groups in one molecule is preferable, and from the viewpoint of good compatibility with the component (A), Further, a cyclic organopolysiloxane having at least two SiH groups in one molecule represented by the following general formula (VI) is preferable.
- R 1 represents an organic group having 1 to 6 carbon atoms, and n represents a number of 3 to 10).
- the substituent R 1 in the compound represented by the general formula (VI) is preferably composed of C, H and O, more preferably a hydrocarbon group, and still more preferably a methyl group.
- the compound represented by the general formula (VI) is preferably 1,3,5,7-tetramethylcyclotetrasiloxane from the viewpoint of availability.
- the molecular weight of the component (B) is not particularly limited, but is preferably low molecular weight from the viewpoint of easier expression of fluidity and easy mixing with powders such as the components (E) and (F). Used.
- the molecular weight is preferably 50 to 100,000, more preferably 50 to 1,000, and still more preferably 50 to 700.
- the viscosity is preferably 50 Pa ⁇ s or less, more preferably 20 Pa ⁇ s or less, and further preferably 5 Pa ⁇ s or less at 23 ° C. It is.
- the viscosity can be measured with an E-type viscometer.
- a component can be used individually by 1 type or in combination of 2 or more types.
- an organic compound ( ⁇ ) containing at least one carbon-carbon double bond reactive to SiH group in one molecule (hereinafter referred to as “ ⁇ component”) And a compound obtained by hydrosilylation reaction of a compound ( ⁇ ) having at least two SiH groups in one molecule.
- ⁇ component an organic compound ( ⁇ ) containing at least one carbon-carbon double bond reactive to SiH group in one molecule
- ⁇ component an organic compound obtained by hydrosilylation reaction of a compound ( ⁇ ) having at least two SiH groups in one molecule.
- the component ( ⁇ ) is the same as the above-described organic compound (A), which is the same as the organic compound containing at least two carbon-carbon double bonds reactive to the SiH group in one molecule (hereinafter “ ( ⁇ 1) component ”) can also be used.
- the component ( ⁇ 1) is used, the resulting resin cured body has a high crosslink density and is likely to be a resin cured body having high mechanical strength.
- an organic compound ( ⁇ 2) (hereinafter referred to as “ ⁇ 2 component”) containing one carbon-carbon double bond reactive to SiH group in one molecule can be used.
- ⁇ 2 component an organic compound containing one carbon-carbon double bond reactive to SiH group in one molecule
- the component ( ⁇ 2) is not particularly limited as long as it is an organic compound containing one carbon-carbon double bond having a reactivity with the SiH group in one molecule, but the component (B) relative to the component (A)
- the compounds containing siloxane units (Si—O—Si) such as polysiloxane-organic block copolymers and polysiloxane-organic graft copolymers are not constituents such as C, H, N, A compound containing only O, S, and halogen is preferable.
- the bonding position of the carbon-carbon double bond having reactivity to the SiH group is not particularly limited, and may be present anywhere in the molecule.
- the compound as the component ( ⁇ 2) can be classified into a polymer compound and a monomer compound.
- the polymer compound include polysiloxane, polyether, polyester, polyarylate, polycarbonate, saturated hydrocarbon, unsaturated hydrocarbon, polyacrylate ester, polyamide, phenol-formaldehyde (Phenol resin type), polyimide type compound, etc. are mentioned.
- monomeric compounds include, for example, aromatic hydrocarbons such as phenols, bisphenols, benzene, and naphthalene: aliphatic hydrocarbons such as straight-chain and alicyclics: heterocyclic compounds; silicone-based compounds Compounds; mixtures thereof; and the like.
- the carbon-carbon double bond having reactivity with the SiH group in the component ( ⁇ 2) is not particularly limited.
- a group represented by the formula: CH 2 ⁇ CH— is particularly preferable.
- the carbon-carbon double bond having reactivity to the SiH group may be directly bonded to the skeleton of the ( ⁇ 2) component, or may be covalently bonded via a divalent or higher substituent.
- the divalent or higher valent substituent is not particularly limited as long as it is a substituent having 0 to 10 carbon atoms.
- the constituent element is C. , H, N, O, S, and those containing only halogen are preferred.
- substituents include divalent or higher valent groups represented by the following [Chemical 26] and [Chemical 27].
- two or more of these divalent or higher valent substituents may be connected by a covalent bond to constitute one divalent or higher valent substituent.
- Examples of the group covalently bonded to the skeleton as described above include vinyl group, allyl group, methallyl group, acrylic group, methacryl group, 2-hydroxy-3- (allyloxy) propyl group, 2-allylphenyl group, 3 -Allylphenyl group, 4-allylphenyl group, 2- (allyloxy) phenyl group, 3- (allyloxy) phenyl group, 4- (allyloxy) phenyl group, 2- (allyloxy) ethyl group, 2,2-bis (allyl) Examples thereof include an oxymethyl) butyl group, 3-allyloxy-2, 2-bis (allyloxymethyl) propyl group, and groups represented by the following [Chemical Formula 28].
- component ( ⁇ 2) examples include propene, 1-butene, 1-pentene, 1-hexene, 1-heptene, 1-octene, 1-nonene, 1-decene, 1-dodecene, 1-undecene, and Idemitsu Petroleum.
- Chains such as Chemical Corporation linearene, 4,4-dimethyl-1-pentene, 2-methyl-1-hexene, 2,3,3-trimethyl-1-butene, 2,4,4-trimethyl-1-pentene
- Aliphatic hydrocarbon compounds cyclohexene, methylcyclohexene, methylenecyclohexane, norbornylene, ethylidenecyclohexane, vinylcyclohexane, camphene, carene, ⁇ -pinene, ⁇ -pinene and other cyclic aliphatic hydrocarbon compounds, styrene, ⁇ -methylstyrene, Indene, phenylacetylene, 4-ethynyltoluene, allylbenzene, 4-phenyl- -Aromatic hydrocarbon compounds such as butene, allyl ethers such as alkyl allyl ether and allyl phenyl ether, glycerin monoallyl
- Aliphatic compounds aromatic compounds such as 1,2-dimethoxy-4-allylbenzene, o-allylphenol, substituted isocyanurates such as monoallyl dibenzyl isocyanurate, monoallyl diglycidyl isocyanurate, vinyl Examples thereof include silicon compounds such as trimethylsilane, vinyltrimethoxysilane, and vinyltriphenylsilane.
- component ( ⁇ 2) examples include polyether resins such as one-end allylated polyethylene oxide and one-end allylated polypropylene oxide, hydrocarbon resins such as one-end allylated polyisobutylene, and one-end allylated polybutyl.
- polyether resins such as one-end allylated polyethylene oxide and one-end allylated polypropylene oxide
- hydrocarbon resins such as one-end allylated polyisobutylene
- one-end allylated polybutyl examples include polymers or oligomers having a vinyl group at one end, such as acrylic resins such as acrylate and one-end allylated polymethyl methacrylate.
- the structure of the ( ⁇ 2) component may be linear or branched, and the molecular weight is not particularly limited, and various types can be used.
- the molecular weight distribution is not particularly limited, the molecular weight distribution is preferably 3 or less, more preferably 2 or less, in that the viscosity of the thermosetting resin composition tends to be low and the moldability tends to be good. Preferably it is 1.5 or less.
- the molecular weight distribution (ratio between the weight average molecular weight and the number average molecular weight) was calculated by a standard polystyrene conversion method using gel permeation chromatography (GPC). However, a GPC column packed with polystyrene cross-linked gel (shodex GPC K-804, K-802.5, manufactured by Showa Denko KK) was used, and chloroform was used as the GPC solvent.
- Tg is preferably 100 ° C. or less in that the obtained resin cured body tends to be tough. More preferably, it is 50 degrees C or less, More preferably, it is 0 degrees C or less.
- preferred resins include polybutyl acrylate resins.
- Tg is preferably 100 ° C. or higher, more preferably 120 ° C. or higher, further preferably 150 ° C. or higher, and most preferably, in terms of increasing the heat resistance of the obtained cured resin. It is 170 ° C or higher.
- Tg can be obtained as a temperature at which tan ⁇ is maximum in the dynamic viscoelasticity measurement.
- the ( ⁇ 2) component is preferably a hydrocarbon compound from the viewpoint of increasing the heat resistance of the obtained cured resin.
- the preferred carbon number is 7-10.
- the ( ⁇ 2) component may have other reactive groups.
- the reactive group in this case include an epoxy group, an amino group, a radical polymerizable unsaturated group, a carboxyl group, an isocyanate group, a hydroxyl group, and an alkoxysilyl group.
- an epoxy group is preferable from the viewpoint that the adhesiveness can be further increased.
- Specific examples include monoallyl diglycidyl isocyanurate, allyl glycidyl ether, allyloxyethyl methacrylate, allyloxyethyl acrylate, and vinyltrimethoxysilane.
- the ( ⁇ 1) component as described above can be used singly or in combination of two or more.
- the component ( ⁇ 2) can also be used alone or in combination of two or more.
- the component ( ⁇ ) is a compound having at least two SiH groups in one molecule, and chain and / or cyclic polyorganosiloxanes are also examples. Specifically, for example, the following compounds represented by [Chemical 29] and [Chemical 30] can be mentioned.
- a cyclic polyorganosiloxane having at least three SiH groups in one molecule represented by the following general formula (VI) is preferable.
- the substituent R 1 in the compound represented by the following general formula (VI) is preferably a group composed of C, H, and O, more preferably a hydrocarbon group, and still more preferably a methyl group. .
- 1,3,5,7-tetramethylcyclotetrasiloxane is preferable.
- R 1 represents an organic group having 1 to 6 carbon atoms
- n represents a number of 3 to 10
- Other examples of the component ( ⁇ ) include compounds having a SiH group such as bisdimethylsilylbenzene.
- the various ( ⁇ ) components described above can be used alone or in combination of two or more.
- a compound obtained by subjecting the ( ⁇ ) component and the ( ⁇ ) component to a hydrosilylation reaction can be used as the (B) component.
- a mixture containing one or more other compounds may be obtained together with the compound that can be used as the (B) component of the present invention.
- Such a mixture can be used as the component (B) as it is without separating the compound that can be used as the component (B) from the mixture to produce the thermosetting resin composition of the present invention.
- the hydrosilylation reaction between the ( ⁇ ) component and the ( ⁇ ) component is specifically as follows.
- the mixing ratio of the ( ⁇ ) component and the ( ⁇ ) component is not particularly limited, but when considering the strength of the cured resin obtained by hydrosilylation of the obtained (B) component and (A) component, Since it is preferable that there are more SiH groups, the total number of carbon-carbon double bonds (X) having reactivity to SiH groups in the generally mixed ( ⁇ ) component and the total number of SiH groups in the mixed ( ⁇ ) component.
- the ratio (Y / X) to (Y) is preferably Y / X ⁇ 2, more preferably Y / X ⁇ 3. Further, from the viewpoint that the compatibility of the component (B) with the component (A) is likely to be improved, preferably 10 ⁇ Y / X, and more preferably 5 ⁇ Y / X.
- component (B) which is a hydrosilylation reaction product of the component ( ⁇ ) and the component ( ⁇ ) include a reaction product of bisphenol A diallyl ether and 1,3,5,7-tetramethylcyclotetrasiloxane, vinyl Reaction product of cyclohexene and 1,3,5,7-tetramethylcyclotetrasiloxane, reaction product of divinylbenzene and 1,3,5,7-tetramethylcyclotetrasiloxane, dicyclopentadiene and 1,3,5,7 -Reactant of tetramethylcyclotetrasiloxane, reaction product of triallyl isocyanurate and 1,3,5,7-tetramethylcyclotetrasiloxane, diallyl monoglycidyl isocyanurate and 1,3,5,7-tetramethylcyclotetra A reaction product of siloxane, allyl glycidyl ether and 1,3,5,7-tetramethylcyclote Reaction product
- the combination of the component (A) and the component (B) is exemplified by at least one selected from the components (A) exemplified above and the above ( B) Various combinations of at least one selected from the components can be mentioned.
- the mixing ratio of the component (A) and the component (B) is not particularly limited as long as the required strength is not lost, but the number of SiH groups (Y) in the component (B) is the carbon in the component (A).
- the ratio (Y / X) to the number of carbon double bonds (X) is preferably 0.3 ⁇ Y / X ⁇ 3, more preferably 0.5 ⁇ Y / X ⁇ 2, and even more preferably 0.7 ⁇ Y / X ⁇ 1.5. When it deviates from the preferred range, sufficient strength may not be obtained or thermal deterioration may easily occur.
- the component (C) of the present invention is a hydrosilylation catalyst.
- the hydrosilylation catalyst is not particularly limited as long as it has catalytic activity for the hydrosilylation reaction.
- a hydrosilylation catalyst can be used individually by 1 type or in combination of 2 or more types.
- the addition amount of the hydrosilylation catalyst is not particularly limited, but in order to have sufficient curability and keep the cost of the thermosetting resin composition relatively low, the amount of SiH group of component (B) is 1 mol. And preferably 10 ⁇ 8 mol to 10 ⁇ 1 mol, more preferably 10 ⁇ 6 mol to 10 ⁇ 2 mol.
- a co-catalyst can be used together with the hydrosilylation catalyst. The kind and amount of the cocatalyst are also the same as the hydrosilylation reaction for obtaining the component (A) and the hydrosilylation reaction for obtaining the component (B).
- the component (D) of the present invention is a silicone compound containing at least one carbon-carbon double bond having reactivity to the SiH group in one molecule.
- a thermosetting resin composition (X) that gives a cured resin body having a smaller linear expansion coefficient can be obtained.
- the silicone compound of component (D) is a compound whose skeleton is substantially formed of Si—O—Si bonds, and various compounds such as linear, cyclic, branched, and partial networks are available. Used. Various substituents may be bonded to such a skeleton.
- Examples of the substituent bonded to the skeleton include alkyl groups such as a methyl group, an ethyl group, a propyl group, and an octyl group, an aryl group such as a phenyl group, a 2-phenylethyl group, and a 2-phenylpropyl group, a methoxy group, an ethoxy group, Examples include an alkoxy group such as an isopropoxy group and a group such as a hydroxyl group.
- a methyl group, a phenyl group, a hydroxyl group, and a methoxy group are preferable, and a methyl group and a phenyl group are more preferable in that heat resistance tends to be high.
- substituent having a carbon-carbon double bond that is reactive to the SiH group include a vinyl group, an allyl group, an acryloxy group, a methacryloxy group, an acryloxypropyl group, and a methacryloxypropyl group.
- a vinyl group is preferable in terms of good reactivity.
- the component (D) may be a compound represented by the following formula.
- R n (CH 2 ⁇ CH) m SiO (4-nm) / 2 (In the formula, R is a group selected from a hydroxyl group, a methyl group or a phenyl group, and n and m are numbers satisfying 0 ⁇ n ⁇ 4, 0 ⁇ m ⁇ 4, and 0 ⁇ n + m ⁇ 4)
- component (D) examples include polydimethylsiloxane having a vinyl group as a terminal group or side chain group, polydiphenylsiloxane, polymethylphenylsiloxane, and two or three random or block copolymers selected from these siloxanes. Examples thereof include polymers, 1,3-divinyltetramethyldisiloxane, 1,3,5,7-tetravinylcyclotetrasiloxane.
- a component can be used individually by 1 type or in combination of 2 or more types.
- linear polysiloxanes having vinyl groups at the ends are preferable, linear polysiloxanes having vinyl groups at both ends are more preferable, and both ends are more preferable in that the effects of the present invention are more easily obtained.
- a linear polymethylphenylsiloxane having a vinyl group is more preferable, and a linear polymethylphenylsiloxane having a vinyl group at both ends, wherein the amount of phenyl groups with respect to all substituents is 20 mol% or more. It is particularly preferred that
- the molecular weight of the component (D) is preferably 1,000 or more and 1,000,000 or less, more preferably 5,000 or more and 100,000 or less, and still more preferably, as the weight average molecular weight (Mw). 10,000 or more and 100,000 or less.
- Mw weight average molecular weight
- the amount of component (D) used is preferably 30% by weight or more, more preferably 50% by weight or more, and still more preferably 80% by weight or more based on the total amount of component (A) and component (B). .
- the mixing ratio of the component (A), the component (B), and the component (D) is not particularly limited as long as the required strength is not lost, but the number of SiH groups (Y) in the component (B) (
- the ratio of the number of carbon-carbon double bonds (X) having reactivity to SiH groups in component A) and component (D) is preferably 0.3 ⁇ Y / X ⁇ 3, more preferably 0 0.5 ⁇ Y / X ⁇ 2, more preferably 0.7 ⁇ Y / X ⁇ 1.5.
- Component (E) of the present invention is an inorganic filler.
- the component (E) has an effect of increasing the strength and hardness of the obtained cured resin or reducing the linear expansion coefficient.
- the inorganic filler of the component (E) various inorganic fillers that are generally used and / or proposed as fillers for conventional epoxy-based sealing materials are used.
- quartz, fumed silica, Silica-based inorganic fillers such as precipitated silica, silicic anhydride, fused silica, crystalline silica, ultrafine amorphous silica, alumina, zircon, silicon nitride, aluminum nitride, silicon carbide, glass fiber, alumina fiber, carbon fiber,
- Examples include mica, graphite, carbon black, graphite, diatomaceous earth, white clay, clay, talc, aluminum hydroxide, calcium carbonate, potassium titanate, calcium silicate, inorganic balloon, silver powder, and the like.
- the inorganic filler is preferably low radiation from the viewpoint of hardly damaging the semiconductor element.
- the inorganic filler may be appropriately surface treated.
- Examples of the surface treatment include treatment with a coupling agent, alkylation treatment, trimethylsilylation treatment, and silicone treatment.
- the coupling agent in this case is a silane coupling agent.
- the silane coupling agent is not particularly limited as long as it is a compound having at least one functional group reactive with an organic group and one hydrolyzable silicon group in the molecule.
- the group reactive with the organic group is preferably at least one functional group selected from an epoxy group, a methacryl group, an acrylic group, an isocyanate group, an isocyanurate group, a vinyl group, and a carbamate group from the viewpoint of handling. From the viewpoints of adhesion and adhesiveness, an epoxy group, a methacryl group, and an acrylic group are particularly preferable.
- As the hydrolyzable silicon group an alkoxysilyl group is preferable from the viewpoint of handleability, and a methoxysilyl group and an ethoxysilyl group are particularly preferable from the viewpoint of reactivity.
- Preferred silane coupling agents include 3-glycidoxypropyltrimethoxysilane, 3-glycidoxypropyltriethoxysilane, 2- (3,4-epoxycyclohexyl) ethyltrimethoxysilane, 2- (3,4- Epoxycyclohexyl) alkoxysilanes having an epoxy functional group such as ethyltriethoxysilane: 3-methacryloxypropyltrimethoxysilane, 3-methacryloxypropyltriethoxysilane, 3-acryloxypropyltrimethoxysilane, 3-acryloxypropyl Methacrylic or acrylic groups such as triethoxysilane, methacryloxymethyltrimethoxysilane, methacryloxymethyltriethoxysilane, acryloxymethyltrimethoxysilane, acryloxymethyltriethoxysilane Such as alkoxysilanes having a group.
- an inorganic compound is added to the thermosetting resin composition used in the present invention and reacted in the thermosetting resin composition or in a partial reaction product of the thermosetting resin composition, and in the thermosetting resin composition And a method of generating an inorganic filler.
- inorganic compounds include hydrolyzable silane monomers or oligomers such as alkoxysilanes, acyloxysilanes, and halogenated silanes, metal alkoxides such as titanium and aluminum, acyloxides, and halides.
- silica-based inorganic fillers are used from the viewpoint that the curing reaction is difficult to inhibit, the effect of reducing the linear expansion coefficient is large, and the adhesion to the lead or the lead frame is likely to be high. preferable. Furthermore, from the viewpoint that the balance of physical properties such as moldability and electrical characteristics is good, fused silica is preferable, from the viewpoint that the thermal conductivity of the cured resin body tends to be high, and a resin molded body design with high heat dissipation becomes possible. Is preferably crystalline silica. Alumina is preferable from the viewpoint that heat dissipation is likely to be higher.
- titanium oxide is preferable from the viewpoint that the light reflectance of the resin used for the resin molded body is high and the light extraction efficiency in the obtained light-emitting device tends to be high.
- glass fiber, potassium titanate, and calcium silicate are preferable from the viewpoint that the reinforcing effect is high and the strength of the resin molded body tends to be high.
- the average particle size and particle size distribution of the inorganic filler various types are used without particular limitation, including those used and / or proposed as fillers for conventional sealing materials such as epoxy type,
- the average particle size usually used is from 0.1 ⁇ m to 120 ⁇ m, and preferably from 0.5 ⁇ m to 60 ⁇ m, more preferably from 0.5 ⁇ m to 15 ⁇ m, from the viewpoint of easy flowability.
- the specific surface area of the inorganic filler can also be variously set, including those used and / or proposed as fillers for conventional sealing materials such as epoxy.
- the shape of the inorganic filler various types such as a crushed shape, a piece shape, a spherical shape, and a rod shape are used.
- Various aspect ratios are used. From the viewpoint that the strength of the obtained cured resin is likely to be high, those having an aspect ratio of 10 or more are preferable.
- a powder form is preferable to a fiber form. From the viewpoint that the flowability at the time of molding tends to improve even during high filling, a spherical shape is preferred.
- the various inorganic fillers described above can be used singly or in combination of two or more.
- the usage-amount of (E) component is not specifically limited, It is preferable that the total amount of (E) component which occupies for the whole thermosetting resin composition (X) is 70 weight% or more, and is 80 weight% or more. More preferably, it is more preferably 90% by weight or more. When the amount of the component (E) is small, it is difficult to obtain the effect of improving the strength and hardness, the effect of reducing the coefficient of linear expansion, and the like.
- the order of mixing the inorganic filler of the component (E) various methods can be used, but from the viewpoint that the storage stability of the intermediate raw material of the thermosetting resin composition (X) tends to be good, A method of mixing the component (A) with the component (C) and the inorganic filler and the component (B) is preferable.
- the component (B) is present in the presence and / or absence of the component (C). Since the components have reactivity with moisture and / or inorganic fillers in the environment, they may be altered during storage. Further, from the viewpoint that the reaction components (A), (B) and (C) are well mixed and a stable molded product is easily obtained, the components (A), (B) and (C ) It is preferable to mix the component and the inorganic filler.
- the inorganic filler of component (E) various means conventionally used and / or proposed for epoxy resins and the like can be used.
- a two-roll, three-roll, planetary stirring and defoaming device, a homogenizer, a dissolver, a planetary mixer and other stirrers, a plast mill and other melt kneaders, and the like can be mentioned.
- a three-roll, melt-kneader is preferable.
- the mixing of the inorganic filler may be performed at normal temperature or may be performed by heating.
- the thermosetting resin composition (X) desirably contains the component (F).
- the component (F) is a white pigment and has an effect of increasing the light reflectance of the obtained cured resin.
- Various components can be used as the component (F), for example, titanium oxide, zinc oxide, magnesium oxide, antimony oxide, zirconium oxide, strontium oxide, niobium oxide, boron nitride, barium titanate, zinc sulfide, barium sulfate. , Magnesium carbonate, inorganic hollow particles, and the like.
- the inorganic hollow particles include sodium silicate glass, aluminum silicate glass, borosilicate soda glass, and shirasu.
- titanium oxide or zinc oxide is preferable from the viewpoint of ease of handling, availability, and cost.
- titanium oxide which may be anatase type or rutile type, but has no photocatalytic action and the thermosetting resin composition (X) becomes stable.
- the rutile type is preferable in that it is easy.
- a method for producing titanium oxide those produced by any method such as sulfuric acid method and chlorine method can be used.
- the average particle size of the component (F) is not particularly limited, and various types can be used, but the light reflectance of the obtained cured resin is likely to be high, and the tablet of the thermosetting resin composition (X) is From the viewpoint of becoming harder, it is preferably 1 ⁇ m or less, more preferably 0.3 ⁇ m or less, and still more preferably 0.25 ⁇ m or less.
- the tablet of the thermosetting resin composition (X) will be described later.
- the fluidity of the thermosetting resin composition (X) is high, it is preferably 0.05 ⁇ m or more, more preferably 0.1 ⁇ m or more.
- the average particle diameter can be measured using a laser diffraction / scattering particle size distribution analyzer.
- the component may be surface-treated.
- the surface of the component (F) is coated with at least one selected from an inorganic compound and an organic compound.
- inorganic compounds include aluminum compounds, silicon compounds, zirconium compounds, tin compounds, titanium compounds, and antimony compounds.
- organic compounds include polyhydric alcohols, alkanolamines or derivatives thereof, and organic siloxanes. Examples thereof include organosilicon compounds, higher fatty acids and metal salts thereof, and organometallic compounds.
- the surface of the component is coated with an inorganic compound or an organic compound using a known method such as a wet method or a dry method, for example, when dry pulverizing, wet pulverizing or slurrying titanium oxide. Can do.
- a wet method or a dry method for example, when dry pulverizing, wet pulverizing or slurrying titanium oxide.
- a liquid phase method and a gas phase method there are various methods such as a liquid phase method and a gas phase method.
- the cured resin obtained is preferably treated with an organosiloxane from the viewpoint of high light reflectance and good heat resistance and light resistance.
- an organic siloxane-treated titanium oxide it is possible to obtain an excellent light-emitting device that has high light extraction efficiency and does not decrease light extraction efficiency even when used for a long period of time.
- organic siloxane treating agents can be used, and examples thereof include silane coupling agents, hexamethyldisiloxane, and hexamethyldisilazane.
- silane coupling agent examples thereof include silane coupling agents, hexamethyldisiloxane, and hexamethyldisilazane.
- silane coupling agent examples thereof include silane coupling agents, hexamethyldisiloxane, and hexamethyldisilazane.
- silane coupling agent can be used as the silane coupling agent.
- polysiloxanes such as polydimethylsiloxane, polymethylphenylsiloxane, polymethylhydrogensiloxane, and copolymers of two or more thereof, hexamethylcyclotrisiloxane , Cyclosiloxanes such as heptamethylcyclotetrasiloxane, 1,3,5,7-tetramethylcyclotetrasiloxane, chlorosilanes such as trimethylchlorosilane, dimethyldichlorosilane, methyltrichlorosilane, 3-glycidoxypropyltrimethoxysilane Epoxy such as 3-glycidoxypropyltriethoxysilane, 2- (3,4-epoxycyclohexyl) ethyltrimethoxysilane, 2- (3,4-epoxycyclohexyl) ethyltriethoxysilane Silanes having functional groups, 3-methacryloxypropyltrime
- organosiloxane treating agents those not containing a carbon-carbon double bond are preferred. When a carbon-carbon double bond is included, the heat resistance tends to be lowered. Moreover, it is also possible to use together surface treating agents other than organosiloxane. Examples of such a surface treatment agent include Al, Zr, and Zn.
- the component (F) may be surface-treated with an inorganic compound.
- the surface treatment method using an inorganic compound is not particularly limited, and various surface treatment methods using an aluminum compound, a silicon compound, a zirconium compound, and the like can be given.
- Various methods can be applied as the surface treatment method, and various methods such as a wet method, a dry method, a liquid phase method, and a gas phase method can be exemplified.
- Titanium oxide may be surface-treated with an inorganic compound or an organic compound for the purpose of improving durability, improving affinity with a medium, and preventing the collapse of particle shape.
- thermosetting resin composition (X) By subjecting the component (F) to a surface treatment with an inorganic compound, the affinity with each component contained in the thermosetting resin composition (X) is improved, and the thermosetting resin composition (X) as the component (F). It is considered that the dispersibility of the resin is improved and the strength of the cured resin body is improved.
- the usage-amount of (F) component is not specifically limited, It is preferable that the quantity of (F) component which occupies for the whole thermosetting resin composition (X) is 10 weight% or more, and is 15 weight% or more. Is more preferable, and it is further more preferable that it is 20 weight% or more. If it is less than 10% by weight, the light reflectance of the resulting cured resin may be lowered.
- the total amount of the component (E) and the component (F) is not particularly limited, but the total amount of the component (E) and the component (F) in the entire thermosetting resin composition (X) is 85% by weight or more. Is preferable, and more preferably 90% by weight or more. When the total amount of the component (E) and the component (F) is small, it is difficult to obtain the effect of increasing the strength and hardness and the effect of reducing the linear expansion coefficient.
- thermosetting resin composition (X) desirably contains a component (G).
- the component (G) is a metal soap and is added to improve moldability including mold release properties of the thermosetting resin composition (X).
- (G) Component includes various conventionally used metal soaps.
- the metal soap here is generally a combination of chain fatty acids and metal ions, and a nonpolar or low polarity part based on fatty acids and a polar part based on a metal binding part are combined in one molecule.
- chain fatty acids include saturated fatty acids having 1 to 18 carbon atoms, unsaturated fatty acids having 3 to 18 carbon atoms, and aliphatic dicarboxylic acids. Among these, saturated fatty acids having 1 to 18 carbon atoms are preferable from the viewpoint of easy availability and high industrial feasibility, and further from the viewpoint of high effect of releasability, 6-18 saturated fatty acids are more preferred.
- metal ions include ions of alkali metals, alkaline earth metals, zinc, cobalt, aluminum, strontium, and the like.
- metal soaps include lithium stearate, lithium 12-hydroxystearate, lithium laurate, lithium oleate, lithium 2-ethylhexanoate, sodium stearate, sodium 12-hydroxystearate, lauric acid Sodium, sodium oleate, sodium 2-ethylhexanoate, potassium stearate, potassium 12-hydroxystearate, potassium laurate, potassium oleate, potassium 2-ethylhexanoate, magnesium stearate, magnesium 12-hydroxystearate, Magnesium laurate, magnesium oleate, magnesium 2-ethylhexanoate, calcium stearate, calcium 12-hydroxystearate, calcium laurate , Calcium oleate, calcium 2-ethylhexanoate, barium stearate, barium 12-hydroxystearate, barium laurate, zinc stearate, zinc 12-hydroxystearate, zinc laurate, zinc oleate, 2-ethyl Examples include zinc hexanoate, lead
- metal stearates are preferable from the viewpoints of easy availability, high safety, and high industrial feasibility. Particularly, from the viewpoint of economy, calcium stearate and stearic acid are preferred. Most preferred is one or more selected from the group consisting of magnesium and zinc stearate.
- the amount of metal soap added is not particularly limited, but is preferably 0.01 to 5 parts by weight, more preferably 0.025 parts by weight to 100 parts by weight of the entire thermosetting resin composition (X).
- the amount is 4 parts by weight, more preferably 0.05 to 4 parts by weight.
- thermosetting resin composition (X) can be added to the thermosetting resin composition (X).
- any of various additives used in a resin cured body for a surface-mounted light-emitting device can be used, for example, a curing retarder, an adhesion improver, an anti-aging agent, a radical inhibitor, an ultraviolet absorber. , Solvents, additives for light emitting elements, release agents and the like.
- the curing retarder can be used, for example, for the purpose of improving the storage stability of the thermosetting resin composition (X) or adjusting the reactivity of the hydrosilylation reaction in the production process.
- the curing retarder include a compound containing an aliphatic unsaturated bond, an organic phosphorus compound, an organic sulfur compound, a nitrogen-containing compound, a tin compound, and an organic peroxide.
- Examples of the compound containing an aliphatic unsaturated bond include 3-hydroxy-3-methyl-1-butyne, 3-hydroxy-3-phenyl-1-butyne, 1-ethynyl-1-cyclohexanol, and other propargyl alcohols.
- Maleic esters such as ene-yne compounds and dimethyl malate.
- Examples of the organophosphorus compound include triorganophosphine, diorganophosphine, organophosphon, and triorganophosphite.
- Examples of the organic sulfur compound include organomercaptans, diorganosulfides, hydrogen sulfide, benzothiazole, thiazole, benzothiazole disulfide and the like.
- Nitrogen-containing compounds include ammonia, primary to tertiary alkylamines, arylamines, urea, hydrazine and the like.
- tin compounds include stannous halide dihydrate and stannous carboxylate.
- organic peroxide include di-tert-butyl peroxide, dicumyl peroxide, benzoyl peroxide, and t-butyl perbenzoate.
- curing retarders from the viewpoint of good retarding activity and good raw material availability, benzothiazole, thiazole, dimethyl malate, 3-hydroxy-3-methyl-1-butyne, 1-ethynyl-1 -Cyclohexanol is preferred.
- the addition amount of the curing retarder can be variously set, but is preferably 10 ⁇ 1 mol to 10 3 mol, more preferably 1 mol to 50 mol, relative to 1 mol of the hydrosilylation catalyst as component (C).
- adhesion improver examples include commonly used adhesives, various coupling agents, epoxy compounds, phenol resins, coumarone-indene resins, rosin ester resins, terpene-phenol resins, ⁇ -methylstyrene-vinyltoluene.
- adhesion improver examples include copolymers, polyethylmethylstyrene, and aromatic polyisocyanates.
- Examples of coupling agents include silane coupling agents and titanate coupling agents. Examples and preferred examples of the coupling agent are the same as those described above. These coupling agents can be used alone or in combination of two or more.
- the amount of coupling agent added can be variously set, but is preferably 0.1 to 50 parts by weight, more preferably 0.5 parts per 100 parts by weight of the total amount of component (A) and component (B). Parts by weight to 25 parts by weight. If the addition amount is small, the effect of improving the adhesiveness does not appear, and if the addition amount is large, the physical properties of the obtained cured resin may be adversely affected.
- epoxy compound examples include novolak phenol type epoxy resin, biphenyl type epoxy resin, dicyclopentadiene type epoxy resin, bisphenol F diglycidyl ether, bisphenol A diglycidyl ether, and 2,2′-bis (4-glycidyloxycyclohexyl).
- the addition amount of the epoxy compound is preferably 1 part by weight to 50 parts by weight, more preferably 3 parts by weight to 25 parts by weight with respect to 100 parts by weight of the total amount of the components (A) and (B). If the addition amount is small, the effect of improving adhesiveness does not appear, and if the addition amount is large, the physical properties of the cured resin may be adversely affected.
- a silanol condensation catalyst can be further used in order to enhance the effect of the coupling agent and the epoxy compound. Thereby, the adhesiveness can be improved and / or stabilized.
- a silanol condensation catalyst is not particularly limited, but is preferably at least one selected from the group consisting of boron compounds, aluminum compounds and titanium compounds.
- Examples of the aluminum compound used as the silanol condensation catalyst include aluminum alkoxides such as aluminum triisopropoxide, sec-butoxyaluminum diisoflopoxide, aluminum trisec-butoxide, ethyl acetoacetate aluminum diisopropoxide, aluminum tris ( Aluminum chelates such as ethyl acetoacetate), aluminum chelate M (manufactured by Kawaken Fine Chemicals, alkyl acetoacetate aluminum diisopropoxide), aluminum tris (acetylacetonate), aluminum monoacetylacetonate bis (ethylacetoacetate), etc. Can be mentioned. From the viewpoint of handleability, aluminum chelates are more preferable.
- Titanium compounds used as silanol condensation catalysts include tetraalkoxy titaniums such as tetraisopropoxy titanium and tetrabutoxy titanium: titanium chelates such as titanium tetraacetylacetonate: general residues having residues such as oxyacetic acid and ethylene glycol And titanate coupling agents.
- Examples of the boron compound serving as a silanol condensation catalyst include boric acid esters.
- boric acid ester those represented by the following general formulas (VII) and (VIII) can be preferably used.
- B (OCOR 1 ) 3 (VIII) (Wherein R 1 represents an organic group having 1 to 48 carbon atoms)
- boric acid esters include tri-2-ethylhexyl borate, normal trioctadecyl borate, trinormal octyl borate, triphenyl borate, trimethylene borate, tris (trimethylsilyl) borate, trinormal butyl borate, boron
- Examples include tri-sec-butyl acid, tri-tert-butyl borate, triisopropyl borate, trinormal propyl borate, triallyl borate, triethyl borate, trimethyl borate, boron methoxyethoxide, and the like.
- These boric acid esters may be used alone or in a combination of two or more. Mixing may be performed in advance, or may be performed at the time of producing the cured resin.
- trimethyl borate triethyl borate, and tri-butyl borate are preferable, and trimethyl borate is more preferable among them from the viewpoint of easy availability and high industrial practicality.
- normal trioctadecyl borate, trinormal octyl borate, triphenyl borate, trimethylene borate, tris (trimethylsilyl) borate, trinormal butyl borate, tri-borate sec-butyl, tri-tert-butyl borate, triisopropyl borate, tri-propyl borate, triallyl borate, methoxy ethoxide borate are preferred, among which normal trioctadecyl borate, tri-tert-butyl borate More preferred are triphenyl borate and trinormal butyl borate.
- trinormal butyl borate, triisopropyl borate and trinormal propyl borate are preferable, and trinormal butyl borate is more preferable.
- trimethyl borate and triethyl borate are preferable, and trimethyl borate is more preferable.
- the amount of the silanol condensation catalyst used can be variously set, but is preferably 0.1 to 50 parts by weight, more preferably 1 to 30 parts by weight with respect to 100 parts by weight of the coupling agent and / or epoxy compound. is there. If the addition amount is small, the effect of improving adhesiveness does not appear, and if the addition amount is large, the physical properties of the cured resin may be adversely affected. These silanol condensation catalysts can be used alone or in combination of two or more.
- a silanol source compound can be further used in order to further enhance the effect of improving adhesiveness.
- the adhesiveness can be improved and / or stabilized.
- silanol source compounds include silanol compounds such as triphenylsilanol and diphenyldihydroxysilane, and alkoxysilanes such as diphenyldimethoxysilane, tetramethoxysilane, and methyltrimethoxysilane. These silanol source compounds can be used singly or in combination of two or more.
- the amount of the silanol source compound used can be variously set, but is preferably 0.1 to 50 parts by weight, more preferably 1 to 30 parts by weight with respect to 100 parts by weight of the coupling agent and / or epoxy compound. is there. If the addition amount is small, the effect of improving the adhesiveness does not appear, and if the addition amount is large, the physical properties of the obtained cured resin may be adversely affected.
- carboxylic acids and acid anhydrides can be used in order to enhance the effect of the coupling agent or epoxy compound. Thereby, the adhesiveness can be improved and / or stabilized.
- carboxylic acids and acid anhydrides are not particularly limited, but each carboxylic acid represented by the following [Chemical Formula 32], 2-ethylhexanoic acid, cyclohexanecarboxylic acid, cyclohexanedicarboxylic acid, methylcyclohexanedicarboxylic acid, tetrahydrophthalate Acid, methyl tetrahydrophthalic acid, methyl hymic acid, norbornene dicarboxylic acid, hydrogenated methyl nadic acid, maleic acid, acetylenedicarboxylic acid, lactic acid, malic acid, citric acid, tartaric acid, benzoic acid, hydroxybenzoic acid, cinnamic acid, phthalic acid Examples thereof include acids, trimellitic
- carboxylic acids and acid anhydrides from the viewpoint of having hydrosilylation reactivity, less possibility of bleeding from the cured resin, and hardly impairing the physical properties of the obtained cured resin, Those containing a carbon-carbon double bond that is reactive with the compound are preferred.
- Preferred carboxylic acids and / or acid anhydrides include, for example, carboxylic acids and tetrahydrophthalic acids represented by the formula: CH 2 ⁇ CH (CH 2 ) n COOH (where n represents a number of 0 to 30). , Methyltetrahydrophthalic acid, single acid anhydrides thereof, complex acid anhydrides thereof and the like.
- the amount of carboxylic acids and / or acid anhydrides used can be variously set, but is preferably 0.1 to 50 parts by weight, more preferably 1 part by weight with respect to 100 parts by weight of the coupling agent and / or epoxy compound. Parts to 10 parts by weight. If the addition amount is small, the effect of improving adhesiveness does not appear, and if the addition amount is large, the physical properties of the cured resin may be adversely affected.
- the above-mentioned silane compound can be used for the thermosetting resin composition (X) of the present invention.
- the silane compound contributes to improving the adhesion with the lead and is effective in preventing moisture from entering from the interface between the cured resin and the lead.
- Specific examples of such silane compounds include dimethyldimethoxysilane, dimethyldiethoxysilane, diphenyldimethoxysilane, diphenyldiethoxysilane, methylphenyldimethoxysilane, and methylphenyldiethoxysilane. preferable.
- anti-aging agent examples include citric acid, phosphoric acid, sulfur-based anti-aging agent, etc., in addition to the anti-aging agents generally used such as hindered phenol type.
- hindered phenol-based anti-aging agent various types such as Irganox 1010 available from Ciba Specialty Chemicals are used.
- Sulfur-based antioxidants include mercaptans, mercaptan salts, sulfide carboxylates, sulfides including hindered phenol sulfides, polysulfides, dithiocarboxylates, thioureas, thiophosphates, sulfonium Examples thereof include compounds, thioaldehydes, thioketones, mercaptals, mercaptols, monothioacids, polythioacids, thioamides, and sulfoxides. These anti-aging agents can be used alone or in combination of two or more.
- radical inhibitors examples include 2,6-di-tert-butyl-3-methylphenol (BHT), 2,2′-methylene-bis (4-methyl-6-tert-butylphenol), tetrakis (methylene- Phenolic radical inhibitors such as 3 (3,5-di-tert-butyl-4-hydroxyphenyl) propionate) methane, phenyl- ⁇ -naphthylamine, ⁇ -naphthylamine, N, N′-secondary butyl-p- Examples include amine radical inhibitors such as phenylenediamine, phenothiazine, N, N′-diphenyl-p-phenylenediamine. These radical inhibitors can be used singly or in combination of two or more.
- UV absorber examples include 2 (2′-hydroxy-3 ′, 5′-di-tert-butylphenyl) benzotriazole, bis (2,2,6,6-tetramethyl-4-piperidine) sebacate and the like. Is mentioned.
- An ultraviolet absorber can be used individually by 1 type or in combination of 2 or more types.
- thermosetting resin composition (X) can be dissolved in a solvent and used.
- Solvents that can be used are not particularly limited, and specific examples include hydrocarbon solvents such as benzene, toluene, hexane, heptane, tetrahydrofuran, 1,4-dioxane, 1,3-dioxolane, diethyl ether, and the like.
- An ether solvent such as acetone, a ketone solvent such as acetone, methyl ethyl ketone, and methyl isobutyl ketone, and a halogen solvent such as chloroform, methylene chloride, and 1,2-dichloroethane can be preferably used.
- toluene, tetrahydrofuran, 1,3-dioxolane, and chloroform are preferable. These solvents can be used alone or in combination of two or more.
- the amount of the solvent used can be appropriately set, but is preferably 0.1 mL to 10 mL with respect to 1 g of the thermosetting resin composition (X) to be used. If the amount used is small, it is difficult to obtain the effect of using a solvent such as a low viscosity, and if the amount used is large, the solvent will remain in the material and easily cause problems such as thermal cracks. It is disadvantageous and the industrial utility value decreases.
- Additives for light emitting elements are used, for example, to improve various characteristics of the light emitting elements.
- additives include phosphors such as yttrium, aluminum, and garnet phosphors activated by cerium that absorb light from the light emitting element to emit longer wavelength fluorescence, and blue that absorbs a specific wavelength.
- Coloring agents such as ing agents, diffusion materials such as titanium oxide, aluminum oxide, melamine resin, CTU guanamine resin, benzoguanamine resin for diffusing light, metal oxides such as aluminosilicate, aluminum nitride, boron nitride, etc. Examples thereof include thermally conductive fillers such as metal nitrides.
- These additives can be used alone or in combination of two or more. Moreover, these additives may be contained uniformly or may be contained with a gradient in content.
- the mold release agent is used to improve the mold release property at the time of molding the thermosetting resin composition (X).
- the release agent include the component (G) already described and waxes.
- waxes include natural wax, synthetic wax, oxidized or non-oxidized polyolefin, and polyethylene wax. In addition, it is better not to use a release agent when sufficient release properties can be obtained without adding a release agent.
- thermosetting resin compositions (X) include colorants, flame retardants, flame retardant aids, surfactants, antifoaming agents, emulsifiers, leveling agents, anti-fogging agents, and ion trapping agents such as antimony-bismuth. , Thixotropic agent, tackifier, storage stability improver, ozone degradation inhibitor, light stabilizer, thickener, plasticizer, reactive diluent, antioxidant, heat stabilizer, conductivity enhancer , Antistatic agents, radiation blocking agents, nucleating agents, phosphorus peroxide decomposing agents, lubricants, pigments, metal deactivators, thermal conductivity-imparting agents, physical property modifiers, etc. Can be added in a range.
- thermoplastic resins can be added to the thermosetting resin composition (X) for the purpose of modifying the characteristics.
- Various thermoplastic resins can be used.
- polymethylmethacrylate resins such as homopolymers of methyl methacrylate, random, block or graft polymers of methyl methacrylate and other monomers (for example, Hitachi Chemical Co., Ltd.) Optretz, etc.), homopolymers of butyl acrylate, random butyl acrylate and other monomers, acrylic resins typified by polybutyl acrylate resins such as block or graft polymers; bisphenol A, 3, 3, Polycarbonate resins such as polycarbonate resin containing 5-trimethylcyclohexylidenebisphenol as a monomer structure (for example, APEC manufactured by Teijin Limited); homoborn or copolymerization of norbornene derivatives, vinyl monomers, etc.
- Cycloolefin resins such as resins obtained by ring-opening metathesis polymerization of norbornene derivatives, and hydrogenated products thereof (for example, APEL manufactured by Mitsui Chemicals, ZEONOR, ZEONEX manufactured by Nippon Zeon, ARTON manufactured by JSR, etc.); ethylene and Olefin-maleimide resins such as maleimide copolymers (eg, TI-PAS manufactured by Tosoh Corporation); bisphenols such as bisphenol A and bis (4- (2-hydroxyethoxy) phenyl) fluorene; and diols such as diethylene glycol Polyester resins such as polyester obtained by polycondensation of phthalic acids and aliphatic dicarboxylic acids such as terephthalic acid and isophthalic acid (eg O-PET manufactured by Kanebo Co., Ltd.); polyethersulfone resins; polyarylate resins; polyvinyl acetal resins Polyethylene resin; polypropylene resin;
- the thermoplastic resin may have a carbon-carbon double bond and / or a SiH group having reactivity to the SiH group in the molecule.
- the molecule has one or more carbon-carbon double bonds and / or SiH groups having reactivity to SiH groups in the molecule on average. Preferably it is.
- the thermoplastic resin may have other crosslinkable groups.
- the crosslinkable group include an epoxy group, an amino group, a radical polymerizable unsaturated group, a carboxyl group, an isocyanate group, a hydroxyl group, and an alkoxysilyl group. From the viewpoint that the heat resistance of the obtained cured resin is likely to be high, it is preferable to have one or more crosslinkable groups on average in one molecule.
- the molecular weight of the thermoplastic resin is not particularly limited, but the number average molecular weight is preferably 10,000 or less, more preferably 5000 or less, from the viewpoint that compatibility with the component (A) or the component (B) is likely to be good. is there. On the contrary, the number average molecular weight is preferably 10,000 or more, more preferably 100,000 or more from the viewpoint that the obtained cured resin is easily tough.
- the molecular weight distribution is not particularly limited, but the molecular weight distribution is preferably 3 or less, more preferably 2 or less, and still more preferably from the viewpoint that the thermosetting resin composition (X) tends to have low viscosity and good moldability. Is 1.5 or less.
- the amount of the thermoplastic resin used is not particularly limited, but is preferably 5% to 50% by weight, more preferably 10% to 30% by weight of the entire thermosetting resin composition (X).
- the addition amount is small, the resulting cured resin body tends to be brittle, and when the addition amount is large, the heat resistance (elastic modulus at high temperature) tends to be low.
- a thermoplastic resin can be used individually by 1 type or in combination of 2 or more types.
- the thermoplastic resin may be dissolved in the component (A) and / or the component (B) and mixed in a uniform state, pulverized and mixed in a particle state, or dissolved in a solvent and mixed. Then, it may be in a dispersed state. From the viewpoint that the obtained cured resin is more likely to be transparent, it is preferable to dissolve in the component (A) and / or the component (B) and mix in a uniform state. Also in this case, the thermoplastic resin may be directly dissolved in the component (A) and / or the component (B), or may be mixed uniformly using a solvent or the like, and then the solvent is removed and uniform dispersion is performed. It is good also as a state and / or a mixed state.
- the average particle diameter can be variously set, but is preferably 10 nm to 10 ⁇ m.
- the average particle diameter may be variously set, but is preferably 10 nm to 10 ⁇ m.
- thermosetting resin particles may be mixed in the thermosetting resin composition (X).
- the thermosetting resin particles can be obtained by curing and pulverizing the thermosetting resin.
- the average particle diameter can be variously set, but is preferably 10 nm to 10 ⁇ m.
- the coefficient of variation of the particle diameter is 10% or less.
- thermosetting resin composition (X) is prepared by, for example, mixing the essential components (A) to (E) described above, and (F) to (G) and other optional components according to the method described above. Can be prepared.
- the thermosetting resin composition (X) thus obtained can be used as it is as a liquid or paste.
- the thermosetting resin composition (X) may be used after mixing each component, additive, etc., and then partially reacting (B-stage) by heating or the like. Viscosity can be adjusted by using the B stage, and transfer moldability can also be adjusted. In addition, there is an effect of further suppressing curing shrinkage.
- thermosetting resin composition (X) preferably has fluidity at a temperature of 150 ° C. or lower from the viewpoint of good moldability by transfer molding or the like.
- the curability of the thermosetting resin composition (X) can be arbitrarily set, but from the viewpoint that the molding cycle can be shortened, the gelation time at 120 ° C. is preferably within 120 seconds, and within 60 seconds. It is more preferable that Further, the gelation time at 150 ° C. is preferably within 60 seconds, and more preferably within 30 seconds. Further, the gelation time at 100 ° C. is preferably within 180 seconds, and more preferably within 120 seconds.
- the gelation time in this case can be measured as follows. An aluminum foil having a thickness of 50 ⁇ m is placed on a hot plate adjusted to a preset temperature, and 100 mg of the thermosetting resin composition (X) is placed on the aluminum foil, and the time until gelation is measured to obtain the gelation time.
- the weight loss during curing is preferably 5% by weight or less, more preferably 3% by weight or less, and even more preferably 1% by weight or less.
- the weight reduction during curing was performed by increasing the temperature of a sample (thermosetting resin composition (X)) 10 mg from room temperature to 150 ° C. at a rate of 10 ° C./min using a thermogravimetric analyzer, It can be determined as a ratio of the reduced weight to the initial weight.
- the content of Si atoms in the volatile component is preferably 1% or less from the viewpoint of hardly causing a problem of silicone contamination.
- thermosetting resin composition (X) preferably contains an N element for the following reason. Electrical and electronic parts are generally required to have flame retardancy. Conventionally, halogen-based flame retardants have been mainly used, but they have been shifted to non-halogen-based flame retardants in order to reduce environmental impact. In addition, environmentally friendly flame retardants are also desired in terms of regulations in the electrical industry, such as RoHS (Restriction of Hazardous Substances) compliance.
- RoHS Restriction of Hazardous Substances
- non-halogen flame retardant containing a phosphinic acid metal salt and an organic phosphorus flame retardant described in JP 2010-77333 A, triazine, guanidine, cyanurate and the like described in JP-T-2007-514828.
- Non-halogen flame retardant comprising at least one nitrogen-containing flame retardant selected from the group consisting of isocyanurates, phosphinic acid salts or diphosphinic acid salts and / or polymers thereof, and char-forming polymers, JP 2002-128969
- An amine salt produced by reacting an amine compound containing at least one nitrogen atom and at least one acid selected from phosphoric acid, pyrophosphoric acid, condensed phosphoric acid and cyanuric acid, , Tris (2-hydroxyethyl) isocyanurate and an isocyanate compound
- Nitrogen compounds are one of the promising non-halogen flame retardants. Therefore, also in the resin molding of this invention, it is preferable to contain a nitrogen atom especially in a resin component.
- a skeleton incorporating an isocyanurate skeleton which is a main skeleton as a nitrogen-based flame retardant is particularly preferable.
- Nitrogen-containing organic compounds such as thiazole and thiazole also act as reaction retarders in the hydrosilylation curing reaction. Therefore, by adding these nitrogen compounds to the thermosetting resin composition that gives the resin molded body, sufficient storage stability can be imparted to the thermosetting resin, and the thermosetting resin composition is completely cured. be able to. Also from such a viewpoint, it is preferable that the resin component contains a nitrogen atom.
- nitrogen-containing organic compounds such as tributylamine, tetramethylethylenediamine, and benzotriazole, which are conventionally known reaction control agents for hydrosilylation reactions, may coexist.
- the method for obtaining the N content in the thermosetting resin composition is not particularly limited, but the N atom or nitrogen-containing organic compound incorporated in the resin skeleton is measured by 14 N-NMR or 14 N-solid NMR. N atoms can be detected.
- the N content in the thermosetting resin composition is not particularly limited, but is preferably 1000 ppm or more. Including nitrogen-containing inorganic fillers such as boron nitride and aluminum nitride as the filler component has no problem at all, and the flame retarding effect due to the organic component itself containing N atoms and the flame retarding effect due to the inorganic filler containing N atoms. Both can be pulled out.
- the Tg of the cured resin obtained by curing the thermosetting resin composition (X) is preferably 100 ° C. or higher, more preferably 150 ° C. or higher, from the viewpoint of good heat resistance. is there.
- Tg is measured using a dynamic viscoelasticity measuring device (trade name: DVA-200, manufactured by IT Measurement Control Co., Ltd.) and a prismatic test piece of 3 mm ⁇ 5 mm ⁇ 30 mm, and predetermined measurement conditions (tensile mode, measurement frequency 10 Hz). Dynamic viscoelasticity measurement is performed at a strain of 0.1%, a static / power ratio of 1.5, and a temperature rising side degree of 5 ° C./min), and is obtained as a peak temperature of tan ⁇ in the measurement result.
- the extracted ion content from the cured resin is preferably less than 10 ppm, more preferably less than 5 ppm, and still more preferably. It is less than 1 ppm.
- the extracted ion content is examined as follows. 1 g of the cut resin cured body is put in a Teflon (registered trademark) container together with 50 ml of ultrapure water and sealed, and treated under conditions of 121 ° C., 2 atm and 20 hours. The obtained extract was analyzed with an ICP mass spectrometer (trade name: HP-4500, manufactured by Yokogawa Analytical Systems Co., Ltd.), and the obtained Na and K content values were cured as a sample resin. Calculated by converting to the concentration in the body.
- the linear expansion coefficient of the cured resin body is not particularly limited. However, it tends to improve the adhesion to a metal lead frame, etc., and the warpage of a resin molded body in which a curable resin is integrally formed on one side of a metal flat plate. From the viewpoint of suppressing the average linear expansion coefficient from 23 ° C. to 150 ° C., preferably 30 ppm or less, more preferably 20 ppm or less, and even more preferably 10 ppm or less.
- thermosetting resin composition (X) has a light reflectance at 420 nm, 440 nm, and 460 nm after curing (in this specification, the reflectance at a specific wavelength is described as the light reflectance) of 80 R% or more, It is desirable that the light reflectivity retention after the heat resistance test at 180 ° C. for 72 hours (light reflectivity after the heat test / initial light reflectivity ⁇ 100) is 90% or more.
- the light reflectance is preferably 75% or more and more preferably 80% or more in the wavelength band of 420 to 700 nm from the viewpoint that the light extraction efficiency of the light-emitting element tends to be high.
- the light reflectance of the cured resin is determined by the reflection of each wavelength measured at a wavelength of 400 nm to 700 nm (at intervals of 20 nm) using a micro-surface spectral color difference meter (trade name: VSS400, manufactured by Nippon Denshoku Industries Co., Ltd.). Rate.
- the reflectance at a wavelength of 460 nm is set to a light reflectance of 460 nm
- the reflectance at a wavelength of 500 nm is set to a light reflectance of 500 nm.
- the measurement values (reflectance) at the respective wavelengths an average value of measurement values at arbitrary four locations (measurement area 0.1 mm ⁇ ) of the concave opening surface of the resin molded body was adopted.
- the retention ratio of the light reflectance after the heat resistance test (for example, a test in which heating is performed in an oven at 180 ° C. for 72 hours) with respect to the initial light reflectance was obtained by the following formula.
- Retention rate (%) [(light reflectivity after heat test) / (initial light reflectivity)] ⁇ 100
- the retention is preferably 80% or more, more preferably 85% or more, and still more preferably 90% or more.
- the light reflectance at a wavelength of 460 nm of the surface of the molded product obtained by curing the thermosetting resin composition (X) is preferably 90% or more, more preferably 95% or more, still more preferably 97% or more, and particularly preferably. 99% or more.
- thermosetting resin composition (X) can be made into a tablet when it contains at least the component (F) in addition to the components (A) to (E).
- a tablet means a solid that retains a constant shape at room temperature, has substantially no change in shape over time, and does not stick together or become integrated when brought into contact with each other.
- the shape of the tablet is not particularly limited, and includes a columnar shape, a prismatic shape, a disk shape, a spherical shape, and the like, and a general cylindrical shape for transfer molding is preferable.
- At least one of the tablets is a liquid having a viscosity at 23 ° C. of 50 Pa seconds or less (A) and (B), (A) and (B) for curing the component (C). It is characterized by containing the components (E) and (F), which are both powders, and (D).
- the entire thermosetting resin composition (X) can flow when the viscosity of the component (A) and the component (B) is lowered at high temperature, and further, when the heating is continued, the curing reaction proceeds and is desired. It is possible to mold to the shape of
- the molding method is not particularly limited, and a molding method such as transfer molding or compression molding, which is generally used for molding a thermosetting resin composition, can be used.
- a molding method such as transfer molding or compression molding, which is generally used for molding a thermosetting resin composition
- thermosetting resin composition that is the raw material is in the form of a paste or clay, it will not be possible to maintain a constant shape, and it will be attached, integrated, or deformed. The supply to the molding machine becomes very difficult.
- the tablet shape makes it easy to measure, transport, and supply to a molding machine, and can be automated, greatly improving productivity.
- the total proportion of the component (E) and component (F) in the tablet (hereinafter sometimes referred to as “filling rate”) is preferably 70 to 95% by weight.
- the distribution of the (E) component and the (F) component in the filling rate is not particularly limited and can be set freely.
- the filling rate is less than 70% by weight, the thermal expansion coefficient of the obtained resin cured body is increased, causing a problem of dimensional change of the resin molded body, and the obtained thermosetting resin composition (X) is hard. There is a problem that it becomes paste or clay and cannot be tableted.
- the filling rate exceeds 95% by weight, the viscosity of the thermosetting resin composition (X) at a high temperature becomes too high and the moldability is lowered, and the resulting tablet becomes too brittle.
- thermosetting resin composition (X) when at least one of the component (A) and the component (B) is liquid at room temperature, it tends to be in the form of a paste or clay when the filling rate is low. In this case, the tablet does not become a tablet, but the moldability at high temperature tends to be good. On the other hand, when the filling rate is high, since there are few components to be flowed, it tends to be flaky or powdery. These can be compressed into a tablet shape by being compressed, but they tend to have poor fluidity at high temperatures and easily deteriorate moldability. Until now, it has been difficult to achieve both tableting and moldability by simply increasing the filling rate.
- thermosetting resin composition (X) the proportion of the particles of 12 ⁇ m or less in the total powder of the component (E) and the component (F) is 40% by volume or more. It was found that moldability can be achieved.
- the resin molded body of the present invention includes, for example, a step (1) of sandwiching and fixing a plurality of leads with a mold, a step (2) of injecting a liquid thermosetting resin into the mold, It can be manufactured by a manufacturing method including a step (3) of curing the liquid thermosetting resin injected into the mold and a step (4) of demolding the resin molded body from the mold.
- a manufacturing method including a step (3) of curing the liquid thermosetting resin injected into the mold and a step (4) of demolding the resin molded body from the mold.
- the mold there are an upper mold and a lower mold, and the surface corresponding to the concave opening surface of the resin molded body in the upper mold has a predetermined ten-point average roughness (Rz).
- Rz ten-point average roughness
- a mold including an upper mold having an upper mating surface in which an upper concave portion is formed at a predetermined position, a lower mold having a flat lower mating surface, and a resin injection hole is used. A plurality of leads are sandwiched and fixed by the upper mating surface and the lower mating surface.
- step (1) is performed as shown in FIG.
- FIG. 10 is a cross-sectional view schematically showing step (1) in one embodiment of the method for producing a resin molded body according to the present invention.
- the direction extending left and right is the longitudinal direction
- the direction perpendicular to the longitudinal direction in the surface of the lower mating surface 36 of the mold 20 is the width direction.
- FIGS. 11 to 13 The same applies to FIGS. 11 to 13.
- the mold 20 shown in FIG. 10A communicates with the upper mold 30 having the upper mating surface 31, the lower mold 35 having the lower mating surface 36, the resin injection hole, and the resin injection hole.
- a plunger 41 provided in the lower mold 35, a mold heating device (not shown), and a vacuum pump (not shown) are provided.
- the resin injection hole is formed by the second convex portion 34 and the lower mating surface 36 formed on the surface of the upper mating surface 31 when the upper mating surface 31 and the lower mating surface 36 are overlapped. For example, it is illustrated as a resin injection hole 40 in FIG.
- the second convex portion 34 will be described later.
- the upper mold 30 and the lower mold 35 are arranged so that the upper mating surface 31 and the lower mating surface 36 are parallel to each other.
- the upper mold 30 is disposed above the lower mold 35 in the vertical direction, and is supported by a driving unit (not shown) so as to be movable up and down.
- a plurality of first protrusions 32 are formed at predetermined positions on the upper mating surface 31 of the upper mold 30.
- An upper concave portion 33 having a plurality of first convex portions 32 is formed on the upper mating surface 31 of the upper mold 30, and the first convex portions 32 are substantially equal in the vertical direction and the horizontal direction at a predetermined interval. It is preferable that they are formed at intervals.
- the three first protrusions 32 adjacent to each other form an adjacent and communicating internal space, and this internal space corresponds to the three-dimensional shape of the cured resin body to be obtained.
- the front end surface of the middle first protrusion 32 is the first lead in the frame unit 22 (see FIG. 14) constituting the lead frame 21 described later.
- the inner lead portion of the second lead 24 and the inner lead portion of the second lead 24 are positioned.
- the liquid thermosetting resin does not flow into such a contact portion.
- the ten-point average roughness (Rz) of the bottom surface 33a of the upper concave portion 33 is 0.5 ⁇ m or more and 15 ⁇ m or less.
- the range of the ten-point average roughness (Rz) of the bottom surface 33a is preferably 0.5 ⁇ m or more, They are 12 micrometers or less, More preferably, they are 0.5 micrometer or more and 11 micrometers or less, More preferably, they are 0.9 micrometer or more and 10.6 micrometers or less.
- Examples of a method for adjusting the Rz of the bottom surface 33a of the upper concave portion 33 to the above range include an electric discharge machining method described in Japanese Patent No. 3907948. More specifically, in this electric discharge machining method, a metal mold, a metal compound powder, or the like is filled in a female mold of a mold to be subjected to discharge surface treatment, and the material powder in the female mold is formed by the male mold. Using the compacted compact body electrode, a pulsed discharge is generated between the compact body electrode and the female or male mold, and the discharge material discharges the electrode material or electrode material. A substance generated by reaction with energy is deposited on a female or male mold surface, and a discharge surface treatment is performed on the mold surface of the mold.
- a cross-sectional shape is formed on the upper mating surface 31 near the plunger pot 44 provided on the lower mating surface 36.
- a second convex portion 34 is formed which is substantially a right triangle. The second convex portion 34 extends in the width direction of the upper mold 30 on the upper mating surface 31, and the height continuously increases as the first convex portion 32 is approached, and at the position closest to the first convex portion 32.
- the first convex portion 32 has a height slightly smaller than the height.
- the second convex portion 34 and the lower mating surface 36 communicate with the plunger pot 44 to melt the thermosetting resin.
- a runner 42 through which the liquid flows and a resin injection hole 40 following the runner 42 are formed.
- the resin injection hole 40 is formed so that the diameter decreases from the entrance to the exit of the liquid thermosetting resin.
- the resin injection hole 40 is preferably formed in a semicircular cross-sectional shape from the viewpoint of smooth injection of the liquid thermosetting resin into the internal space of the mold 20.
- the runner 42 is configured such that the diameter continuously decreases from the vicinity of the plunger 41 toward the resin injection hole 40, but is not limited thereto, for example, on the upper mating surface 31.
- a runner (not shown) having a certain width may be provided by configuring the lower surface of the second convex portion 34 to be parallel to the lower mating surface 36.
- the lower mold 35 is fixed by support means (not shown).
- the lower mold 35 has a flat lower mating surface 36.
- a through hole 43 in the thickness direction is formed in the lower mold 35, and a plunger 41 is disposed in the through hole 43 so as to be movable up and down by a driving means (not shown).
- the plunger 41 may have a heating means inside.
- the plunger pot 44 is formed by lowering the plunger 41.
- the plunger pot 44 is filled with a thermosetting resin tablet or a liquid thermosetting resin that becomes a liquid thermosetting resin by heating.
- the liquid thermosetting resin in the plunger pot 44 is pressed into the upper concave portion 33 from the resin injection hole 40 through the runner 42 by raising the plunger 41.
- FIG. 14 is a plan view of the frame unit 22 constituting the lead frame 21.
- a plurality of frame units 22 shown in FIG. 14 are arranged in parallel in the width direction and the longitudinal direction, and are integrated.
- the first lead 23, the first lead 23, and the second lead 24 are disposed so as to be separated from each other.
- the material of the lead frame 21 is not particularly limited, but a metal material such as copper is preferable.
- a lead frame in which the first lead 23 and the second lead 24 are printed on the surface of a substrate made of a ceramic material or a plastic material can be used.
- notches are formed vertically and horizontally along the boundary between the frame units 22.
- the notch is sandwiched between the flat surface of the upper mating surface 31 where the first convex portion 32 and the second convex portion 34 are not formed and the lower mating surface 36. Or you may position so that a notch may be pinched
- the notched portion is filled with a liquid thermosetting resin.
- the contact area between the lead frame 21 and the cured resin body 12 is increased, and the adhesion between them is improved.
- a cured resin body is integrally formed on the surface of each frame unit 22 to produce an aggregate of a plurality of resin molded bodies, the thickness of the metal to be cut can be reduced by cutting along the notch. Become. As a result, the resin molded bodies can be easily separated one by one, and the mass productivity is further improved.
- a metal layer such as a plating layer may be formed on at least one surface of the lead frame 21 in the thickness direction.
- the material for the metal layer include gold, silver, copper, and aluminum.
- step (2) a liquid thermosetting resin is injected from the resin injection hole 40 into the molding internal space in the mold 20.
- the molding internal space is formed by the upper recess 33 and the lead frame 21 or the upper recess 33 and the lower mating surface 36.
- step (2) is performed as shown in FIG. FIG. 11: is sectional drawing which shows typically the process (2) in one Embodiment of the manufacturing method of the resin molding which concerns on this invention.
- the lead frame 21 is sandwiched between the upper mating surface 31 and the lower mating surface 36 in the step (1), so that the upper recess 33, the lead frame 21, and the upper frame are placed in the mold 20.
- a molding internal space is formed by the recess 33 and the lower mating surface 36.
- the thermosetting resin tablet 45 with which the plunger 41 and the plunger pot 44 were filled is raised.
- the liquid thermosetting resin 45 obtained by heating the thermosetting resin tablet 45 with the plunger 41 is moved into the mold 20 by further raising the plunger 41 and a vacuum pump (not shown).
- the inner space for molding is filled from the runner 42 through the resin injection hole 40 into the inner space for molding by reducing the inner space for molding.
- a liquid thermosetting resin is also filled in the internal space between the first lead 23 and the second lead 24 in the frame unit 22. Subsequently, the process proceeds to step (3).
- step (3) the liquid thermosetting resin is cured by heating a mold in which a plurality of internal spaces are filled with a liquid thermosetting resin at a predetermined temperature, so that a predetermined position of the lead frame is obtained.
- An assembly of resin molded bodies in which a cured resin body is integrally molded is prepared.
- step (3) is performed as shown in FIG. FIG. 12: is sectional drawing which shows typically the process (3) in one Embodiment of the manufacturing method of the resin molding which concerns on this invention.
- the molding internal space in the mold 20 is filled with a liquid thermosetting resin.
- the mold 20 is heated by the heating means provided in the mold 20.
- the heating temperature and the heating time are appropriately selected according to the curing temperature of the thermosetting resin filled in the internal space.
- a resin molded body assembly 25 in which the cured resin body 12 is integrally formed on the surface of each frame unit 22 constituting the lead frame 21 is obtained.
- Rz of the bottom surface 33a is transferred to the surface of the cured resin body 12 that is in contact with the bottom surface 33a of the upper concave portion 33 (the opening surface of the concave portion 13), and Rz becomes 1 to 10 ⁇ m. Subsequently, the process proceeds to step (4).
- step (4) the resin-cured lead frame 25 is removed from the mold. More specifically, step (4) is performed as shown in FIG. FIG. 13: is sectional drawing which shows typically the process (4) in one Embodiment of the manufacturing method of the resin molding which concerns on this invention.
- step (4) shown in FIG. 13 the upper mold 30 is raised and the lead frame 25 with the cured resin body is taken out of the mold 20, whereby the cured resin body 12 is integrally formed on one surface of the lead frame 21.
- the lead frame 25 with a cured resin body, which is an aggregate of resin molded bodies, is removed from the mold 20.
- the lead frame 25 with a cured resin body which is an assembly of the resin molded bodies, has a dimension range of 40 to 50 mm in length and 40 to 55 mm in width, a lead frame portion thickness of 0.20 mm to 0.30 mm, and a height of the recess. Is preferably 0.10 mm to 0.55 mm, and the warpage after curing is preferably ⁇ 1.0 mm or less.
- the cured resin body from the upper mold 30 Since the Rz of the surface of the resin cured body 12 that is in contact with the bottom surface 33a of the upper concave portion 33 (the opening surface of the concave portion 13) is in the range of 1 ⁇ m to 10 ⁇ m, the cured resin body from the upper mold 30 The releasability of 12 is remarkably improved. Thereby, the deformation
- the releasability of the cured resin body 12 from the upper mold 30 is determined when the above-described thermosetting resin composition (X) is used as the thermosetting resin or thermosetting resin composition that gives the cured resin body 12. , Further significantly improved.
- FIG. 15 is a drawing schematically showing a configuration of a resin molded body obtained by the method for manufacturing a resin molded body according to the present invention.
- 15A is a plan view
- FIG. 15B is a partially enlarged plan view
- FIG. 15C is a partially enlarged sectional view taken along line XX in FIG. 15B.
- the lead frame 25 with the cured resin body is an integrally formed body of the cured resin body 12 and the lead frame 21, and a plurality of recesses 13 are arranged vertically and horizontally, and the first frame constituting the lead frame 21 is formed at the bottom of each recess 13.
- the second lead is exposed through the insulating layer of the cured resin body 12 (not shown). That is, the lead frame 25 with a cured resin body is an aggregate of a plurality of resin molded bodies.
- the lead frame 25 with the cured resin body may be used as it is in the mounting process of the light emitting element, or each resin molded body obtained by cutting it may be used in the mounting process of the light emitting element.
- transfer molding is used as a molding method for producing a resin molded body, but the present invention is not limited to this, and thermoplastic resins such as injection molding, RIM molding, casting molding, press molding, compression molding, etc.
- thermoplastic resins such as injection molding, RIM molding, casting molding, press molding, compression molding, etc.
- Various molding methods generally used for thermosetting resins such as epoxy resins and silicone resins are used.
- transfer molding is preferred in that the molding cycle is short and the moldability is good.
- the molding conditions can be arbitrarily set, for example, the molding temperature is also arbitrary. However, in terms of fast curing and a short molding cycle, the moldability tends to be good, more preferably 100 ° C. or higher, more preferably 120 ° C. or higher. A temperature of 150 ° C. or higher is preferable.
- post-curing After molding by the various methods as described above, post-curing (after-curing) is optional as required. Post-curing tends to improve heat resistance.
- Molding may be performed at a constant temperature, but the temperature may be changed in multiple steps or continuously as necessary. It is preferable that the reaction is carried out while raising the temperature in a multistage or continuous manner, rather than at a constant temperature, in that a uniform cured resin body without distortion can be easily obtained. On the other hand, it is preferable to carry out at a constant temperature in that the molding cycle can be shortened.
- the pressure during molding can be variously set as required, and molding can be performed under normal pressure, high pressure, or reduced pressure. It is preferable to cure under reduced pressure in terms of suppressing the generation of voids, improving the filling property, and easily removing volatile components generated in some cases. On the other hand, in terms of preventing cracks in the molded body, it is preferable to cure under pressure.
- the surface-mounted light-emitting device (hereinafter simply referred to as “light-emitting device”) of the present invention has a resin-cured body and a plurality of leads integrally formed, and has a recess in which the plurality of leads are exposed at the bottom.
- Rz is 1 ⁇ m or more and 10 ⁇ m or less, and it is mounted on a resin molded body having a predetermined glass transition temperature, light reflectance, and light reflectance retention ratio, and on the bottom of the concave portion of the resin molded body, and can be energized with multiple leads.
- a transparent resin layer that seals the light emitting element.
- a plurality of light emitting elements may be mounted on the bottom of the recess of the resin molded body.
- the resin molded body As the resin molded body, the resin cured body and the plurality of leads are integrally molded, and the bottom portion has a recess where the plurality of leads are exposed, and the Rz of the opening surface of the recess is 1 ⁇ m or more It can have the same configuration as a conventional surface mount light emitting device except that a resin molded body having a size of 10 ⁇ m or less is used.
- the resin molded body the above-described various resin molded bodies can be used.
- any conventionally used light emitting element can be used, and examples thereof include a light emitting diode (LED) and a laser diode (LD).
- Examples of the light emitting diode include a blue LED chip, an ultraviolet LED chip, a red LED chip, a green LED chip, and a yellow-green LED chip.
- a chip having a PN junction structure or an NPN junction structure, and two electrodes are horizontal or Includes chips arranged vertically.
- the light emitting element is connected to a plurality of leads so as to be energized by a known connection method such as wire bonding or flip chip bonding.
- a known connection method such as wire bonding or flip chip bonding.
- the light emitting element has two electrodes and the plurality of leads have a first lead and a second lead, one electrode of the light emitting element is connected to the inner side of the first lead. Connecting to the lead portion and connecting the other electrode of the light emitting element to the inner lead portion of the second lead.
- a method of fixing the light emitting element to the bottom of the concave portion of the resin molded body for example, a method of adhering using an adhesive may be mentioned.
- the adhesive for example, silver paste, eutectic solder (AuSn, AuGe, AuSi, etc.), gold bump, or the like is used.
- the melting point of the eutectic solder is preferably in the range of 200 ° C to 350 ° C.
- the pn junction temperature rises, so it is preferable to use eutectic solder, gold bumps, or the like that can provide stable joint strength at high temperatures.
- the light emitting element forms an adhesive layer on the surface of the lead having the plating layer at the bottom of the concave portion of the resin molded body (at this time, the lead and the adhesive layer are electrically connected) and emits light thereon.
- the element is mounted and fixed on the lead surface by heating and melting.
- the adhesive layer can be formed by a general technique such as printing of paste material, dispensing, preform, foil molding, metallization, ball molding, and the like. By providing the adhesive layer made of metal, the heat dissipation of the light emitting device can be improved.
- the flatness of the region where the light emitting element is joined on the lead surface is preferably 0.001 to 50 ⁇ m. Flatness is expressed as the height of the center of the measurement region with respect to the reference surface when a surface including any three corners of the region to be measured is used as the reference surface. If the flatness is less than 0.001 ⁇ m, the surface of the plating layer formed on the lead surface becomes too smooth, the adhesion strength between the plating layer and the adhesive layer is lowered, and the adhesive layer tends to be easily peeled off. is there. Moreover, when flatness exceeds 50 micrometers, the junction area of a plating layer and an adhesive bond layer will become small. As a result, the heat dissipation of the light emitting device tends to decrease, and the bonding strength between the light emitting element and the lead frame tends to decrease.
- any of the transparent resins for sealing conventionally used in surface mounted light emitting devices can be used.
- epoxy resin silicone resin, acrylic resin, urea resin And imide resin.
- SiH as proposed in JP 2002-80733 A and JP 2002-88244 A
- Thermosetting containing an aliphatic organic compound having at least two carbon-carbon double bonds reactive with a group, a compound having at least two SiH groups in one molecule, and a hydrosilylation catalyst It is preferable to use a conductive resin composition as a sealant.
- the transparent resin layer is prepared by injecting a liquid transparent resin into a cup, cavity, package (resin molded body) recess, or the like in which a light emitting element is arranged at the bottom by a dispenser or other methods and curing it by heating or the like.
- the solid or high-viscosity liquid composition may be flowed by heating or the like, injected into the package recess or the like, and further cured by heating or the like.
- the transparent resin can be formed by transfer molding, injection molding or insert molding.
- a lens may be mounted in the concave portion of the resin molded body after the light emitting element is mounted.
- the lens is not particularly limited, and any lens generally used in the field of surface-mounted light-emitting elements can be used, or a transparent resin may be molded into a lens shape.
- the shape of the light-emitting device is not limited, and various shapes used in the field of surface-mounted light-emitting devices can be adopted, but a MAP type in which a cured resin body is attached to one side of a metal lead frame is preferable. By using the MAP type, the effect of the present invention can be easily obtained.
- the light emitting device of the present invention can be used for various known applications. Specifically, for example, backlights such as liquid crystal display devices, illumination, sensor light sources, vehicle instrument light sources, signal lights, indicator lights, display devices, light sources of planar light emitters, displays, decorations, various lights, etc. .
- Glass transition temperature (Tg) Using a surgical knife made by ELP, a resin sample having dimensions of 2 to 5 mm in the longitudinal direction, 0.5 to 1 mm in the width direction, and 0.5 to 1 mm in thickness was cut out from the resin molded body. This sample is put into a thermomechanical analyzer (trade name: TMA, model: TMA / SS6100, manufactured by SII Nanotechnology Co., Ltd.), and the temperature rise / fall rate is in the range of -50 ° C to 250 ° C under nitrogen gas flow. The change in expansion coefficient was measured at 5 ° C./min and a compression load of 29.4 mN, and the glass transition temperature was calculated. Further, the average thermal expansion coefficient of 23 ° C. to 150 ° C. at the time of the above measurement is defined as the average linear expansion coefficient.
- the reflectance at wavelengths of 400 nm to 700 nm (20 nm intervals) was measured to obtain the light reflectance.
- measurement was performed at any four locations (measurement area 0.1 mm ⁇ ) on the concave opening surface of the resin molded body, and the average value of the obtained measurement values was defined as the light reflectance at that wavelength.
- Solid 13 C NMR spectrum A resin sample of 0.5 g was cut out from the resin molding, ground in a mortar, and packed into a 3.2 mm ⁇ solid NMR sample tube. This sample tube was loaded into a VARIAN NMR apparatus (600 MHz), 13 C CP / MAS NMR measurement was performed at a magic angle spinning speed of 20 kHz, and a solid 13 C NMR spectrum of the sample was obtained.
- the resulting solution was heated and stirred as it was for 6 hours, and unreacted 1,3,5,7-tetramethylcyclotetrasiloxane and toluene were distilled off under reduced pressure.
- the obtained compound had a structure represented by the following [Chemical Formula 33] in which a part of the SiH group of 1,3,5,7-tetramethylcyclotetrasiloxane reacted with triallyl isocyanurate by 1 H-NMR measurement. It turns out that it has.
- the unreacted rate of 1,3,5,7-tetramethylcyclotetrasiloxane was 0.8%.
- the total amount of unreacted 1,3,5,7-tetramethylcyclotetrasiloxane, toluene and allyl glycidyl ether by-products is 5,000 ppm or less in total.
- the solution was distilled off under reduced pressure until a colorless and transparent liquid was obtained.
- Example 1 50 parts by weight of the thermosetting resin composition C obtained in the formulation example shown in Table 1, 27 parts by weight of the following (D) component, 557 parts by weight of the following (E) component, and 239 parts by weight of the following (F) component And a thermosetting resin composition (Xa) was prepared. In addition, it weighed so that it might become a total of 100g with the ratio of each said component, and mixed uniformly. The same applies to the following embodiments.
- Component (D) Linear methylphenyl silicone containing vinyl groups at both ends (trade name: PDV2331, manufactured by Gelest, the amount of phenyl groups based on all substituents is 22 to 25 mol%)
- component spherical silica (trade name: MSR-2212? TN, manufactured by Tatsumori Co., Ltd., specific gravity 2.2, average particle size 24.8 ⁇ m, ratio of particles having a particle size of 12 ⁇ m or less: 28%)
- a lead frame made of Cu having a length of 50 mm, a width of 55 mm, and a thickness of 0.25 mm with Ag plating having a thickness of 3 ⁇ m on the surface is prepared.
- the lead frame is an integrally molded product in which the frame units 22 shown in FIG. 14 are arranged in parallel in 15 rows and 12 rows. In each frame unit 22 of the lead frame, 180 resin molded bodies (reflectors) were formed with an interval of 1.1 mm in the vertical and horizontal directions.
- Each resin molding has an inverted frustoconical shape in the interior space of the recess, the diameter of the recess opening surface is 2.1 mm, the diameter of the recess bottom is 1.8 mm, and the inclination angle of the inner wall surface of the recess is 75 with respect to the recess bottom. ° having a height of 0.55 mm, having an insulating portion with a width of about 0.2 mm extending in the vertical direction at 0.45 mm from the right end along the transverse diameter of the bottom of the recess,
- the second leads 23 and 24 were electrically insulated.
- Transfer molding was performed using a G-Line manual press manufactured by Apic Yamada Co., Ltd.
- the mold clamping force was 30 ton
- the injection pressure was 7.7 MPa
- the injection speed was 3 mm / s.
- White compound (thermosetting resin composition (Xa)) (5.0 g) is weighed, shaped into a column to form a tablet, loaded into a plunger pot, and sprayed onto the surface facing the molding inner space of the mold A fluorine-based mold release agent (trade name: Daifree GA-7500, manufactured by Daikin Industries, Ltd.) was applied.
- the molding conditions were 170 ° C./3 minutes and 7.8 to 13.7 MPa.
- Rz of the bottom surface of the upper concave portion formed on the upper mating surface of the upper mold was adjusted to 6.0 ⁇ m.
- a lead frame with a cured resin body is placed on a steel surface plate with a surface roughness (Rz) of 0.8 ⁇ m, flatness of 0.01 mm, and a size of 320 mm ⁇ 212 mm ⁇ 18 mm. Place it toward the surface plate side, apply a straight ruler (Shinwa Measurement Co., Ltd., stainless straight 150 mm) to the gap between the lead frame with a cured resin body and the surface plate, measure the distance of the gap, The warpage value was used.
- a clearance gauge manufactured by Nagai Gauge Manufacturing Co., Ltd., 0.1 mm to 1.0 mm: 0.1 mm interval
- the value of the maximum gauge that could be inserted into the gap was taken as the warp value.
- the value (mm) having the longest distance from the surface plate was taken as the warp value of the lead frame with the cured resin body.
- the case where the resin molded body was concave when viewed from the side was defined as forward warping (+), and the case where it was convex was defined as reverse warping (-).
- thermosetting resin composition D obtained in the formulation example shown in Table 1, 2.81 parts by weight of the following (D) component, 58.23 parts by weight of the following (E) component, and the following (F) component 33.51 parts by weight and 0.20 part by weight of the following component (G) were mixed to prepare a thermosetting resin composition (Xb).
- G component: calcium stearate
- thermosetting resin composition (Xb) obtained above was used instead of the thermosetting resin composition (Xa).
- the resin molded body was not deformed or destroyed due to interface peeling.
- ten-point average roughness (Rz), glass transition temperature (Tg), light reflectance, and solid 13 CNMR spectrum were examined. The results are shown in Table 2.
- Rz ten-point average roughness
- Tg glass transition temperature
- light reflectance and solid 13 CNMR spectrum
- thermosetting organopolyamide (melting point: 76 ° C.) represented by the following formula: Polysiloxane was obtained. (CH 3 ) 1.0 Si (OC 3 H 7 ) 0.06 (OH) 0.11 O 1.4
- thermosetting organopolysiloxane 100 parts by weight of the thermosetting organopolysiloxane obtained above, 100 parts by weight of titanium dioxide (white pigment, rutile type, average particle size 0.3 ⁇ m, trade name: PFC-104, manufactured by Ishihara Sangyo Co., Ltd.), inorganic filling 560 parts by weight of material (spherical fused silica, average particle size 20 ⁇ m, trade name: MSR-200, manufactured by Tatsumori Co., Ltd.), inorganic filler (spherical fused silica, average particle size 0.5 ⁇ m, trade name: Admafine S0- 25R, Admatech Co., Ltd.) 40 parts by weight and a curing catalyst (zinc benzoate, manufactured by Wako Pure Chemical Industries, Ltd.) 3 parts by weight are uniformly melt-mixed in a continuous kneader, cooled and pulverized, and silicone-based thermosetting A functional resin composition was prepared.
- titanium dioxide white pigment
- a resin molded body was produced in the same manner as in Example 1 except that the silicone-based thermosetting resin composition obtained above was used and Rz of the upper concave bottom surface formed in the upper mold was not adjusted. .
- the resin molded body was removed from the upper mold, the resin molded body was deformed or broken.
- the ten-point average roughness (Rz), glass transition temperature (Tg), light reflectance, and solid state 13 CNMR spectrum of the concave opening surface were examined. The results are shown in Table 2.
- the resin molded body is deformed when the resin molded body is removed from the upper mold by adjusting the Rz of the concave opening surface of the resin molded body to be 1 ⁇ m to 10 ⁇ m. And the occurrence of fracture due to interfacial delamination was significantly suppressed. Further, from the comparison between Examples 1 and 2 and Comparative Examples 1 and 2 in Table 2, the light reflectance, heat resistance, and reflection retention were remarkably improved by using the thermosetting resin composition (X). I understand that In addition, Comparative Example 1 shows good light reflectivity, but the glass transition temperature is as low as ⁇ 2 ° C., so that the strength is not sufficient when releasing from the mold, and the cutting associated with the separation of the resin molded body into pieces. When processing, the mechanical strength becomes insufficient, and the quality sufficient as a product, such as chipping of the resin molded portion, is not satisfied.
- thermosetting resin composition (Xa) or (Xb) was press-molded so as to be 170 ° C. ⁇ curing time 2 minutes, mold release rate 0.2 mm / s, sample shape: ⁇ 30 ⁇ thickness 1 mm. The release mode of the molded product when the mold was opened was evaluated.
- the surface condition (unevenness) was observed and evaluated with the naked eye. A surface glossy and smooth surface was indicated by ⁇ , a surface glossy surface and unevenness that could be observed with the naked eye, and a surface glossiness that was low and unevenness could be observed with the naked eye.
- the light reflectance of the molded body surface is higher than that of the molded bodies obtained in Examples 3 to 6 and 7 to 10. It decreased by about 2%. Furthermore, the glossiness decreased by visual observation, and surface irregularities were observed with the naked eye. Thus, the conditions under which a resin molded body having an excellent light reflectance was obtained by defining Rz on the surface of the molded body became clear.
- thermosetting resin compositions (Xc) and (Xd) As shown in Table 6 and Table 7, regardless of the mold roughness, any of the thermosetting resin compositions (Xc) and (Xd) as materials
- the resin molded product also exhibited cohesive failure (CF), inferior releasability and low resin strength, and a satisfactory molded product could not be obtained. Therefore, the glass transition temperature (Tg) could not be measured.
- thermosetting resin composition D 5.25 parts by weight, the following (D) component 2.81 parts by weight, the following (E) component 58.23 parts by weight, the following (F) component 33.51 parts by weight, and the following ( G) 0.20 part by weight of component was mixed, and a thermosetting resin composition (Xb) was prepared in the same manner as in Example 2. Using this thermosetting resin composition (Xb), an assembly of resin molded bodies was produced as follows.
- a Cu lead frame having a length of 50 mm, a width of 55 mm, and a thickness of 0.25 mm is prepared.
- the lead frame is an integrally molded product in which the frame units 22 shown in FIG. 14 are arranged in parallel in 15 rows and 12 rows.
- An Ag plating layer having a thickness of 3 ⁇ m was formed on the surface of the lead frame, and an Au plating layer having a thickness in the range of 0.005 ⁇ m to 0.006 ⁇ m was further formed on the surface of the Ag plating layer.
- 180 resin molded bodies (reflectors) were formed with an interval of 1.1 mm in the vertical and horizontal directions.
- Each resin molding has an inverted frustoconical shape in the interior space of the recess, the diameter of the recess opening surface is 2.1 mm, the diameter of the recess bottom is 1.8 mm, and the inclination angle of the inner wall surface of the recess is 75 with respect to the recess bottom. ° having a height of 0.55 mm, having an insulating portion with a width of about 0.2 mm extending in the vertical direction at 0.45 mm from the right end along the transverse diameter of the bottom of the recess,
- the second leads 23 and 24 were electrically insulated.
- Transfer molding was performed using a compact manual molding device (trade name: G-Line manual system, manufactured by Apic Yamada Co., Ltd.).
- the mold clamping force was 30 ton, the injection pressure was 7.7 MPa, and the injection speed was 3 mm / s.
- White compound (thermosetting resin composition Xb) (5.0 g) is weighed, shaped into a column to form a tablet, loaded into a plunger pot, and sprayed fluorine on the surface facing the molding internal space of the mold A series release agent (trade name: Daifree GA-7500, manufactured by Daikin Industries, Ltd.) was applied.
- the molding conditions were 170 ° C./3 minutes and 7.8 to 13.7 MPa.
- Rz of the bottom surface of the upper concave portion formed on the upper mating surface of the upper mold was adjusted to 6.0 ⁇ m. Further, after the molding, curing was performed at 180 ° C. for 1 hour. When the resin molded body was removed from the upper mold, the resin molded body was not deformed or destroyed due to interface peeling.
- Example 12 A Ni—Pd—Au three-layer plating layer was formed on the surface of a Cu lead frame having a length of 50 mm, a width of 55 mm, and a thickness of 0.25 mm so that the Au plating layer became the outermost surface layer.
- the thickness of the Ni plating layer was in the range of 0.5 to 2.0 ⁇ m.
- the thickness of the Pd plating layer was in the range of 0.01 to 0.15 ⁇ m.
- the thickness of the Au plating layer was in the range of 0.003 to 0.01 ⁇ m.
- a resin molded body aggregate was produced in the same manner as in Example 11 except that this lead frame was used.
- Example 13 Except for using a lead frame made of Cu having a length of 50 mm, a width of 55 mm, and a thickness of 0.25 mm on which an Ag plating layer having a thickness in the range of 2 to 5 ⁇ m is formed, An assembly was produced.
- the resin moldings obtained in Examples 11 to 13 the ten-point average roughness (Rz) of the concave opening surface, the glass transition temperature (Tg), the light reflectance, the initial luminance of the light emitting device mounted with the light emitting element, and use The lead frame was examined for sulfidation resistance. The results are shown in Table 8.
- a silicone-based sealant (OE6630 manufactured by Toray Dow Corning Co., Ltd., a transparent curable resin in which A agent and B agent are mixed at a ratio of 1: 4) is dispensed by a dispenser device to each recess, The part where the light emitting element was mounted was sealed. Thereafter, curing at 150 ° C. for 2 hours was performed to obtain a collective substrate of the surface-mounted light emitting device. This was diced into a size of 30 mm ⁇ 30 mm by a dicing apparatus to obtain an individual surface-mounted light emitting device. The evaluation of the light emission characteristics was performed using a photometric measuring device in accordance with CIE127 (Condition B). Further, the surface-mounted light-emitting device was mounted on a printed circuit board for energization evaluation, a constant current of 20 mA was applied, and the initial luminance (cd: equivalent to candela) at that time was measured.
- OE6630 manufactured by Toray Dow Corning Co., Ltd. a
- the outer peripheral surface 32 b of the first convex portion 32 is divided into a first outer peripheral surface that follows the top surface 32 a of the first convex portion 32 and a second outer peripheral surface that follows the first outer peripheral surface. .
- the inclination angle of the first outer peripheral surface with respect to the top surface 32a is 90 ° (Examples 14 and 15) or 120 ° (Example 16), and the second outer peripheral surface
- the first outer peripheral surface is inclined at 140 ° (Example 14) or 150 ° (Examples 15 and 16) with respect to the top surface 32 (the angle formed by the top surface 32a and the extension line of the second outer peripheral surface).
- the boundary between the first outer peripheral surface and the second outer peripheral surface is a region having a height of 100 ⁇ m (Examples 14 and 15) or 50 ⁇ m (Example 16) from the top surface 32a of the outer peripheral surface 32b.
- the 1st convex part 32 which has the outer peripheral surface 32b which consists of a 1st outer peripheral surface and a 2nd outer peripheral surface, and the 1st convex part 32 which has the outer peripheral surface 32b whose inclination angle with respect to the bottom face 32a is constant at 140 degrees.
- the ten-point average roughness Rz of the bottom surface 33a of the upper concave portion 33 was adjusted to 6.0 ⁇ m.
- the thermosetting resin composition (Xb) is used instead of the thermosetting resin composition (Xa).
- the resin flash burr did not adhere to the frame.
- An assembly of resin molded bodies having recesses having a value (h) shown in FIG. 9 was obtained.
- Example 17 The outer peripheral surface 32b of the first convex portion 32 is not divided into the first outer peripheral surface and the second outer peripheral surface, and the angle formed by the top surface 32a and the outer peripheral surface 32b is 150 ° (Example 17) or 140 ° (implementation).
- a resin molded body with a MAP-shaped lead frame was produced in the same manner as in Example 14 except that Example 18) was used. When the obtained resin molded body was removed from the upper mold, the resin molded body was not deformed or destroyed due to interfacial peeling.
- tilt angle with respect to the bottom face 13a of the inner wall face 13b is a value shown in Table 9 was obtained.
- the interface between the cured resin body and the lead frame and the lead frame exposed at the recesses were visually confirmed.
- the aggregates of the resin molded bodies of Examples 14 to 16 almost no resin chipping and resin burrs were observed. It was.
- the aggregates of the oil and fat molded bodies of Examples 17 and 18 slight resin chipping and resin burrs were visually observed, and further, very fine resin chips and resin burrs were confirmed by optical microscope confirmation.
- the inner wall surface is composed of the second inclined surface having an inclination angle of 45 ° to 90 ° and the first inclined surface having an inclination angle of more than 0 ° and not more than 45 °. It is clear that the formation of the concave portion having a markedly suppressed occurrence of resin chipping or resin burr.
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Abstract
Description
(b)上側合わせ面の凹部とリードフレームおよび/または下側合わせ面とにより形成された内部空間に、樹脂注入孔から液状の熱硬化性樹脂を注入する工程。
(c)金型を加熱することにより、注入された液状の熱硬化性樹脂を硬化させ、樹脂硬化体をリードフレームの所定位置に接着させる工程。
(d)金型を脱型し、リードフレームと樹脂硬化体とが一体成形され、底部にリードフレームが露出する凹部を有する樹脂成形体を得る工程。
(e)凹部の底部に露出するリードフレームに発光素子を通電可能に実装する工程。
(f)凹部に透明性樹脂を充填して発光素子を封止する工程。
1.樹脂硬化体と複数のリードとが一体成形され、底部に複数のリードが露出する凹部を有する表面実装型発光装置用樹脂成形体であって、凹部の開口面の十点平均粗さ(Rz)が1μm以上、10μm以下であり、樹脂硬化体のガラス転移温度が10℃以上であり、ガラス転移温度が、熱機械分析装置(TMA)を用い、温度範囲-50~250℃、昇温速度5℃/分および試料サイズ長1~5mmの条件で測定された値であり、かつ、凹部の開口面の460nmにおける光反射率が80%以上であり、樹脂成形体を180℃で72時間加熱した後の開口面における光反射率の保持率が90%以上である表面実装型発光装置用樹脂成形体。
5.金属層は、最表面層、および、リードの表面と最表面層との間に介在する第2金属層を有し、第2金属層は、Ag層、Pd層又はAg層とPd層との積層体である上記4に記載の表面実装型発光装置用樹脂成形体。
6.金属層がめっき層である上記4または5に記載の表面実装型発光装置用樹脂成形体。
9.第1リードは、凹部の底部に露出する第1インナーリード部と、樹脂硬化体に接触する第1アウターリード部とを含み、かつ、第2リードは、凹部の底部に露出する第2インナーリード部と、樹脂硬化体に接触する第2アウターリード部とを含む上記8に記載の表面実装型発光装置用樹脂成形体。
10.外側面に、第1アウターリード部および/または第2アウターリード部が露出する上記9に記載の表面実装型発光装置用樹脂成形体。
12.第1インナーリード部および第2インナーリード部はその表面に前記金属層を有し、第1アウターリード部および第2アウターリード部はその表面に金属層を有していない上記9~11のいずれかに記載の表面実装型発光装置用樹脂成形体。
13.複数のリードは、樹脂硬化体が充填されている切り欠き部を有する上記1~12のいずれかに記載の表面実装型発光装置用樹脂成形体。
16.上側凹部が上側合わせ面の所定位置に形成された上金型と、平坦な下側合わせ面を有する下金型と、所定の間隔を空けて縦横に切り欠き部が形成された複数のリードと、を用いることにより、複数のリードの切り欠き部で囲まれた領域毎に樹脂硬化体を形成し、次いで切り欠き部に沿って複数のリードを切断することにより、複数個の樹脂成形体を得る上記14または15に記載の表面実装型発光装置用樹脂成形体の製造方法。
18.複数のリードの切り欠き部が、上側合わせ面の上側凹部が形成されていない領域と、下側合わせ面と、により挟持される上記16または17に記載の表面実装型発光装置用樹脂成形体の製造方法。
19.上記1~13のいずれかに記載の表面実装型発光装置用樹脂成形体と、樹脂成形体の凹部底部に実装され、複数のリードと通電可能に接続される発光素子と、発光素子を封止する透明樹脂層と、を備える表面実装型発光装置。
20.複数個の発光素子が実装される上記19に記載の表面実装型発光装置。
本発明の樹脂成形体は、樹脂硬化体と複数のリードとが一体成形され、底部に複数のリードが露出する凹部を有し、凹部の開口面の十点平均粗さ(以下単に「Rz」とすることがある)が1μm以上、10μm以下であることを特徴の一つとする。
本実施形態では、第1リード10および第2リード11という一対のリードを用いているが、これに限定されず、3本以上の任意の数のリードを用いても良い。
樹脂成形体1の立体形状は本実施形態ではほぼ平板状であるが、それに限定されず、発光装置の設計などに応じて各種形状から適宜選択される。
このような構成を採ることによっても、第1リード10および第2リード11を確実に保護し、樹脂成形体4を用いた表面実装型発光装置の信頼性を高めることができる。
さらに、本実施形態においても、樹脂成形体の底部に露出する第1リードおよび第2リードの少なくとも一部にもめっき層を形成してもよい。
(A)成分はSiH基と反応性を有する炭素-炭素二重結合を1分子中に少なくとも2個含有する有機化合物であれば特に限定されない。
有機重合体系化合物である(A)成分としては、たとえば、ポリエーテル系、ポリエステル系、ポリアリレート系、ポリカーボネート系、飽和炭化水素系、不飽和炭化水素系、ポリアクリル酸エステル系、ポリアミド系、フェノール-ホルムアルデヒド系(フェノール樹脂系)、ポリイミド系の骨格を有するものを挙げることができる。
上記一般式(III)のR1は、得られる樹脂硬化体の耐熱性がより高くなりうるという観点からは、好ましくは炭素数1~20の一価の有機基であり、より好ましくは炭素数1~10の一価の有機基であり、さらに好ましくは炭素数1~4の一価の有機基である。これらの好ましいR1の例としては、メチル基、エチル基、プロピル基、ブチル基、フェニル基、ベンジル基、フェネチル基、ビニル基、アリル基、グリシジル基、下記[化15]に例示される各一価基などが挙げられる。
CH2=C(R4)-R3- (V)
〔式中R3は直接結合または炭素数1~48の二価の有機基を表し、R4は水素原子またはメチル基を表す。〕
で表される有機化合物であることがさらに好ましい。
ただし、上記のような一般式(III)で表される有機化合物の好ましい例においても、SiH基に対して反応性を有する炭素-炭素二重結合を1分子中に少なくとも2個含有することは必要である。耐熱性をより向上させるという観点からは、SiH基に対して反応性を有する炭素-炭素二重結合を1分子中に3個以上含有する有機化合物であることがより好ましい。
一般式(VI)で表される化合物中の置換基R1は、好ましくはC、H、O以外の構成元素を含まない基であり、より好ましくは炭化水素基であり、さらに好ましくはメチル基である。また、入手容易性などから、一般式(VI)で表わされる化合物は、1,3,5,7-テトラメチルシクロテトラシロキサンであることが好ましい。
上記したような各種(β)成分は1種を単独でまたは2種以上を組み合わせて使用できる。
このヒドロシリル化反応において、SiH基に対して反応性を有する炭素-炭素二重結合を1分子中に少なくとも2個含有する有機化合物と(β)成分との混合比率は、特に限定されないが、反応中のゲル化が抑制できるという点においては、一般に、前者におけるSiH基に対して反応性を有する炭素-炭素二重結合の総数(X)と後者におけるSiH基の総数(Y)との比が、好ましくはX/Y≧2、より好ましくはX/Y≧3である。また(A)成分の(B)成分に対する相溶性がよくなりやすいという観点からは、好ましくは10≧X/Y、より好ましくは5≧X/Yである。
これらの触媒の中では、触媒活性の観点から塩化白金酸、白金-オレフィン錯体、白金-ビニルシロキサン錯体などが好ましい。また、これらの触媒は1種を単独でまたは2種以上を組み合わせて使用できる。
反応時間、反応時の圧力も必要に応じ種々設定できる。
その他、反応性を制御する目的などのために種々の添加剤を用いてもよい。
(A)成分は、1種を単独でまたは2種以上を組み合わせて使用できる。
(B)成分としては、1分子中に少なくとも2個のSiH基を含有する化合物であれば特に制限がなく、たとえば、国際公開WO96/15194に記載される化合物で、1分子中に少なくとも2個のSiH基を有するものなどが使用できる。
一般式(VI)で表される化合物中の置換基R1は、好ましくはC、H、Oから構成されるものであり、より好ましくは炭化水素基であり、さらに好ましくはメチル基である。また、一般式(VI)で表される化合物としては、入手容易性の観点からは、1,3,5,7-テトラメチルシクロテトラシロキサンであることが好ましい。
(B)成分は、一種を単独でまたは2種以上を組み合わせて使用できる。
重合体系化合物としては、たとえば、ポリシロキサン系、ポリエーテル系、ポリエステル系、ポリアリレート系、ポリカーボネート系、飽和炭化水素系、不飽和炭化水素系、ポリアクリル酸エステル系、ポリアミド系、フェノール-ホルムアルデヒド系(フェノール樹脂系)、ポリイミド系の化合物などが挙げられる。
(β)成分のその他の例として、ビスジメチルシリルベンゼンなどのSiH基を有する化合物が挙げられる。
上記した各種(β)成分は、1種を単独でまたは2種以上を組み合わせて使用できる。
Rn(CH2=CH)mSiO(4-n-m)/2
(式中、Rは水酸基、メチル基あるいはフェニル基から選ばれる基であり、n、mは0≦n<4、0<m≦4、0<n+m≦4を満たす数)
無機充填材の比表面積についても、エポキシ系などの従来の封止材の充填材として使用および/または提案されているものをはじめ、各種設定できる。
上記した各種の無機充填材は、1種を単独でまたは2種以上を組み合わせて使用できる。
(F)成分としては種々のものを用いることができ、たとえば、酸化チタン、酸化亜鉛、酸化マグネシウム、酸化アンチモン、酸化ジルコニウム、酸化ストロンチウム、酸化ニオブ、窒化ホウ素、チタン酸バリウム、硫化亜鉛、硫酸バリウム、炭酸マグネシウム、無機中空粒子などが挙げられる。無機中空粒子としては、たとえば、珪酸ソーダガラス、アルミ珪酸ガラス、硼珪酸ソーダガラス、シラスなどが挙げられる。これらの中でも、取り扱いの容易性や入手性、コストの観点から酸化チタンまたは酸化亜鉛が好ましい。
平均粒径は、レーザー回折散乱式粒度分布計を用いて測定することができる。
(E)成分および(F)成分の合計量が少ないと、強度や硬度を高くする効果や、線膨張率を低減化する効果が得られにくくなる。
(G)成分は金属石鹸であり、熱硬化性樹脂組成物(X)の離型性をはじめとする成形性を改良するために添加される。
B(OR1)3 (VII)
B(OCOR1)3 (VIII)
(式中R1は炭素数1~48の有機基を表す。)
これらのシラノール縮合触媒は1種を単独でまたは2種以上を組み合わせて使用できる。
ヒンダートフェノール系老化防止剤としては、チバスペシャリティーケミカルズ社から入手できるイルガノックス1010をはじめとして、各種のものが用いられる。
これらの老化防止剤は1種を単独でまたは2種以上を組み合わせて使用できる。
熱可塑性樹脂は1種を単独でまたは2種以上を組み合わせて使用できる。
保持率(%)=[(耐熱試験後の光反射率)/(初期の光反射率)]×100
保持率は、電子材料として用いた場合に信頼性が高いといった観点からは、好ましくは80%以上、より好ましくは85%以上、さらに好ましくは90%以上である。
本発明の樹脂成形体は、たとえば、複数のリードを金型で挟持して固定する工程(1)と、金型内に液状の熱硬化性樹脂を注入する工程(2)と、金型内に注入された液状の熱硬化性樹脂を硬化させる工程(3)と、金型から樹脂成形体を脱型する工程(4)を含む製造方法により製造できる。金型としては、上金型と下金型とを有し、上金型における樹脂成形体の凹部開口面に対応する面が所定の十点平均粗さ(Rz)を有する以外は、従来のトランスファモールド成形用金型と同じものを使用できる。以下に、工程(1)~(4)について、詳細に説明する。
上金型30は、下金型35の鉛直方向上方に配置され、図示しない駆動手段により上下動可能に支持されている。上金型30の上側合わせ面31には、複数の第1凸部32が所定の位置に形成されている。上金型30の上側合わせ面31には、複数の第1凸部32を有する上側凹部33が形成され、第1凸部32は、所定の間隔を空けて、縦方向および横方向にほぼ等間隔に形成されていることが好ましい。
リードフレーム21は、上側合わせ面31と下側合わせ面36とを重ねたときに、上側凹部33とフレーム単位22とが所定の位置で重なるように下側合わせ面36に載置される。
本発明の表面実装型発光装置(以下単に「発光装置」とする)は、樹脂硬化体と複数のリードとが一体成形され、底部に複数のリードが露出する凹部を有し、凹部の開口面のRzが1μm以上、10μm以下であり、所定のガラス転移温度、光反射率および光反射率の保持率を有する樹脂成形体と、樹脂成形体の凹部底部に実装され、複数のリードと通電可能に接続される発光素子と、発光素子を封止する透明樹脂層と、を備えている。なお、樹脂成形体の凹部底部には、複数個の発光素子が実装されていても良い。
また、発光素子としては、従来から用いられている発光素子をいずれも使用でき、たとえば、発光ダイオード(LED)、レーザダイオード(LD)などが挙げられる。前記発光ダイオードには、たとえば、青色LEDチップ、紫外線LEDチップ、赤色LEDチップ、緑色LEDチップ、黄緑色LEDチップなどがあり、PN接合構造またはNPN接合構造を有するチップ、2つの電極が水平型または垂直型に配置されるチップなどを含む。
本発明の発光装置は、従来公知の各種の用途に用いることができる。具体的には、たとえば、液晶表示装置などのバックライト、照明、センサー光源、車両用計器光源、信号灯、表示灯、表示装置、面状発光体の光源、ディスプレイ、装飾、各種ライトなどが挙げられる。
樹脂成形体の凹部開口面の十点平均粗さ(Rz)を、輪郭形状測定器(サーフコム500DX、株式会社東京精密製)を用いて、JISB0633:01/ISO04288:96に基づき、触針R:2μmの条件で測定した。
ELP社製手術用メスを用いて、樹脂成形体から、長手方向2~5mm×幅方向0.5~1mm×厚み0.5~1mmの寸法を有する樹脂試料を切り出した。この試料を熱機械分析装置(商品名:TMA、型式:TMA/SS6100、エスアイアイ・ナノテクノロジー(株)製)に投入し、窒素ガスフロー下、-50℃から250℃の範囲を昇降温速度5℃/分、圧縮加重29.4mNで膨張率の変化を測定し、ガラス転移温度を算出した。また、上記測定時の23℃~150℃の平均の熱膨張係数を平均線膨張係数とする。
微小面分光色差計(商品名:VSS400、日本電色工業(株)製)を用い、波長400nm~700nm(20nm間隔)における反射率を測定し、光反射率とした。ここでは、各波長において、樹脂成形体の凹部開口面の任意の4箇所(測定面積0.1mmφ)で測定を行ない、得られた測定値の平均値をその波長における光反射率とした。
また、耐熱試験(180℃のオーブンで72時間加熱する試験)後の光反射率(B)の、初期の光反射率(A)に対する保持率(%)は、下記式により算出した。
保持率(%)=[光反射率(B)/光反射率(A)]×100
樹脂成形体から樹脂試料0.5gを切り出し、乳鉢ですり潰して、3.2mmφの固体NMR試料管に詰めた。この試料管をVARIAN NMR装置(600MHz)に装填し、マジックアングルスピニング速度20kHzで13C CP/MAS NMR測定を実施し、試料の固体13CNMRスペクトルを求めた。
5Lの四つ口フラスコに、攪拌装置、滴下漏斗および冷却管をセットした。このフラスコにトルエン1800gおよび1,3,5,7-テトラメチルシクロテトラシロキサン1440gを入れ、120℃のオイルバス中で加熱および攪拌した。これに、トリアリルイソシアヌレート200g、トルエン200gおよび白金ビニルシロキサン錯体のキシレン溶液(白金として3重量%含有)1.44mlの混合液を50分かけて滴下した。得られた溶液をそのまま6時間加温および攪拌した後、未反応の1,3,5,7-テトラメチルシクロテトラシロキサンおよびトルエンを減圧留去した。得られた化合物は、1H-NMRの測定により、1,3,5,7-テトラメチルシクロテトラシロキサンのSiH基の一部がトリアリルイソシアヌレートと反応した下記[化33]に示す構造を有するものであることがわかった。
2Lオートクレーブにトルエン720gおよび1,3,5,7-テトラメチルシクロテトラシロキサン240gを入れ、気相部を窒素で置換した後、ジャケット温50℃で加熱および攪拌した。これに、アリルグリシジルエーテル171g、トルエン171gおよび白金ビニルシロキサン錯体のキシレン溶液(白金として3重量%含有)0.049gの混合液を90分かけて滴下した。滴下終了後にジャケット温を60℃に上げてさらに40分間反応させ、1H-NMRでアリル基の反応率が95%以上であることを確認した。
表1の内容に従って各成分を配合して、熱硬化性樹脂組成物A~Dを調製した。
表1に示す配合例で得られた熱硬化性樹脂組成物C 50重量部、下記(D)成分27重量部、下記(E)成分557重量部、および下記(F)成分239重量部を均一に混合し、熱硬化性樹脂組成物(Xa)を調製した。なお、前記各成分の比率で、トータル100gになるように秤取り、均一に混合した。以下の実施例でも同様である。
(E)成分:球状シリカ(商品名:MSR?2212?TN、(株)龍森製、比重2.2、平均粒径24.8μm、12μm以下の粒子の割合:28%)
(F)成分:酸化チタン(商品名:タイペークPC?3、石原産業(株)製、ルチル型、比重4.2、塩素法、表面有機:Al、Si、ポリメチルハイドロジェンシロキサン、平均粒径0.21μm、12μm以下の粒子の割合:100%)
厚み3μmのAgメッキを表面に施した縦50mm、横55mm、厚み0.25mmのCu製のリードフレームを準備する。リードフレームは、図14に示すフレーム単位22が縦15列、横12列にわたって平行に並んだ一体成形品である。このリードフレームの各フレーム単位22に、縦横方向の間隔を1.1mmにして樹脂成形体(リフレクター)180個を形成した。各樹脂成形体は、凹部の内部空間の形状が逆円錐台状であり、凹部開口面の径が2.1mm、凹部底部の径が1.8mm、凹部内壁面の凹部底面に対する傾斜角度が75°、高さ0.55mmであり、凹部底部の横方向直径に沿って右端から0.45mmのところに縦方向に延びる幅約0.2mmの絶縁部を有し、フレーム単位22の第1、第2リード23,24を電気的に絶縁していた。
得られた樹脂成形体について、十点平均粗さ(Rz)、ガラス転移温度(Tg)、光反射率および固体13CNMRスペクトルを調べた。結果を表2に示す。
樹脂硬化体付リードフレームを、表面粗さ(Rz)が0.8μm、平面度0.01mm、サイズ320mm×212mm×18mmの鋼鉄製定盤の上に、樹脂硬化体を上側に向け、リードフレームを定盤側に向けて置き、樹脂硬化体付リードフレームと定盤との隙間に対して直定規(シンワ測定株式会社製、ステン直尺 150mm)を直角にあて、その隙間の距離を計測し、反り値とした。または、すきまゲージ(永井ゲージ製作所製、0.1mm~1.0mm:0.1mm間隔)を隙間に差し込んで、隙間に挿入できる最大ゲージの値を反り値とした。樹脂硬化体付リードフレームの4辺のうちで定盤から最も距離がある値(mm)をその樹脂硬化体付リードフレームの反り値とした。樹脂成形体を真横から見た状態で凹になっている場合を順反り(+)、凸になっている場合を逆反り(-)と定義した。
表1に示す配合例で得られた熱硬化性樹脂組成物D 5.25重量部、下記(D)成分2.81重量部、下記(E)成分58.23重量部、下記(F)成分33.51重量部、および下記(G)成分0.20重量部を混合し、熱硬化性樹脂組成物(Xb)を調製した。
(E)成分:シリカ(MSR?2212?TN)
(F)成分:酸化亜鉛(酸化亜鉛1種、比重5.6、平均粒径0.6μm、堺化学工業(株)製)
(G)成分:ステアリン酸カルシウム
なお、実施例1において熱硬化性樹脂組成物Cに代えて表1に示す熱硬化性樹脂組成物AまたはBを用いても、実施例1と同様の結果が得られた。
メチルトリクロロシラン100重量部、トルエン200重量部を1Lのフラスコに入れ、氷冷下で水8重量部およびイソプロピルアルコール60重量部の混合液を、内温を-5~0℃とし、5~20時間かけて液中滴下した。その後、反応混合物を加熱して還流温度で20分間撹拌した。それから室温まで冷却し、水12重量部を30℃以下、30分間で滴下し、20分間撹拌した。更に水25重量部を滴下後、40~45℃で60分間撹拌した。その後水200重量部を加えて有機層を分離した。この有機層を中性になるまで洗浄し、その後共沸脱水、濾過、減圧ストリップをすることにより、下記式で示される無色透明の固体(融点76℃)36.0質量部の熱硬化性オルガノポリシロキサンを得た。
(CH3)1.0Si(OC3H7)0.06(OH)0.11O1.4
市販の白色LED電球(商品名:EVERREDS、パナソニック(株)製)から、発光装置を取り出し、樹脂成形体の十点平均粗さ(Rz)、ガラス転移温度(Tg)、光反射率および固体13CNMRスペクトルを調べた。結果を表2に示す。
また、表2における実施例1および2と、比較例1および2との比較から、熱硬化性樹脂組成物(X)を用いることにより、光反射率、耐熱性および反射保持率が顕著に向上することが分かる。また、比較例1は、良好な光反射率を示すが、ガラス転移温度が-2℃と低いため、金型からの離型時に強度が十分でなく、樹脂成形体の個片化に伴う切削加工をする際、機械的強度が不十分となり、樹脂成形部の欠けなど製品として十分な品質を満たさなくなる。
精密ホットプレス(商品名:CYPF-10、新東工業(株)製)の上下プレス板の上型に、表面ラフネスの異なる金型入子[(十点平均粗さ(Rz)=0.9、2.5、5.8、10.6、15.6(μm)]を装着し、下型に十点平均粗さ(Rz)=0.9の金型を装着した。この装置を用い、熱硬化性樹脂組成物(Xa)または(Xb)を、170℃×硬化時間2分、離型速度0.2mm/s、サンプル形状:φ30×厚み1mmとなるようにプレス成形した。その後、金型をオープンした際の成形物の剥離モードを評価した。
実施例3~6および比較例3の結果を表3に示す。実施例7~10および比較例4の結果を表4に示す。
このように成形体表面のRzを規定することで、優れた光反射率を有する樹脂成形体が得られる条件が明らかとなった。
下記表5に示す各成分を、表5に示す配合割合で均一に混合し、熱硬化性樹脂組成物(Xc)および(Xd)を調製した。
実施例3~10および比較例3~4と同様の条件で、次のようにしてプレス成形を実施した。精密ホットプレス(CYPF-10)の上下プレス板の上型に、表面ラフネスの異なる金型入子[(十点平均粗さ(Rz)=0.9、2.5、5.8、10.6、15.6(μm)]を装着し、下型に十点平均粗さ(Rz)=0.9の金型を装着した。この装置を用い、熱硬化性樹脂組成物(X)を、170℃×硬化時間2分、離型速度0.2mm/s、サンプル形状:φ30×厚み1mmとなるようにプレス成形した。その後、金型をオープンした際の成形物の剥離モードを評価し、また固体13CNMRスペクトルを評価した。参考例1~5の結果を表6に示し、参考例6~10の結果を表7に示す。
熱硬化性樹脂組成物D:5.25重量部、下記(D)成分2.81重量部、下記(E)成分58.23重量部、下記(F)成分33.51重量部、および下記(G)成分0.20重量部を混合し、実施例2と同様にして、熱硬化性樹脂組成物(Xb)を調製した。この熱硬化性樹脂組成物(Xb)を用い、下記のようにして樹脂成形体の集合体を作製した。
(E)成分:シリカ(MSR-2212-TN)
(F)成分:酸化亜鉛(酸化亜鉛1種、比重5.6、平均粒径0.6μm、堺化学工業(株)製)
(G)成分:ステアリン酸カルシウム
縦50mm、横55mm、厚み0.25mmのCu製のリードフレームを準備する。リードフレームは、図14に示すフレーム単位22が縦15列、横12列にわたって平行に並んだ一体成形品である。このリードフレーム表面に厚み3μmのAgめっき層を形成し、さらにAgめっき層の表面に厚み0.005μm~0.006μmの範囲でAuめっき層を形成した。このリードフレームの各フレーム単位22に、縦横方向の間隔を1.1mmにして樹脂成形体(リフレクター)180個を形成した。各樹脂成形体は、凹部の内部空間の形状が逆円錐台状であり、凹部開口面の径が2.1mm、凹部底部の径が1.8mm、凹部内壁面の凹部底面に対する傾斜角度が75°、高さ0.55mmであり、凹部底部の横方向直径に沿って右端から0.45mmのところに縦方向に延びる幅約0.2mmの絶縁部を有し、フレーム単位22の第1、第2リード23,24を電気的に絶縁していた。
縦50mm、横55mm、厚み0.25mmのCu製リードフレームの表面に、Auめっき層が最表面層になるように、Ni-Pd-Auの3層めっき層を形成した。Niめっき層の厚みは0.5~2.0μmの範囲とした。Pdめっき層の厚みは0.01~0.15μmの範囲とした。Auめっき層の厚みは0.003~0.01μmの範囲とした。このリードフレームを用いる以外は、実施例11と同様にして、樹脂成形体の集合体を作製した。
厚みが2~5μmの範囲であるAgめっき層を表面に形成した縦50mm、横55mm、厚み0.25mmのCu製のリードフレームを用いる以外は、実施例11と同様にして、樹脂成形体の集合体を作製した。
実施例11~13で得られた樹脂成形体について、凹部開口面の十点平均粗さ(Rz)、ガラス転移温度(Tg)、光反射率、発光素子を実装した発光装置の初期輝度および使用したリードフレームの耐硫化性を調べた。結果を表8に示す。
上記で得られた樹脂成形体の集合体(リードフレーム付き樹脂成形体)の各凹部に、ダイボンダー装置及びエポキシ性ダイボンド剤(商品名:DX-20C、ヘンケル社製)を用いて、発光素子(商品名:B1213、Genetits社製)を接合し、ワイヤーボンダー装置により各凹部の底部に露出する第1、第2インナーリード部と発光素子とを結線した。続いて、各凹部に対し、シリコーン系封止剤(東レ・ダウコーニング社製OE6630、A剤およびB剤をそれぞれ1:4の割合で混合した透明硬化性樹脂)をディスペンサ―装置によりディスペンスし、発光素子がマウントされた部位を封止した。その後、150℃2時間のキュアを実施し、表面実装型発光装置の集合基板を得た。これを、ダイシング装置により30mm×30mmのサイズにダイシングして、個片化された表面実装型発光装置を得た。発光特性の評価は、光度測定装置を使用し、CIE127(ConditionB)に準拠して実施した。また、表面実装発光装置を通電評価用プリント基板に実装し、定電流20mAを通電しその時の初期輝度(cd:カンデラ相当)を計測した。
Agめっき、Au-AgめっきおよびAu-Pd-Niめっきを施したCu製のリードフレームの耐硫化性を次の手法で評価した。あらかじめのリードフレーム表面の光沢度(値)を計測しておいた。続いてビーカー(1L)に純水200mL、多硫化硫黄含有成分(商品名:湯の素、村上商会製)を5mL入れ、マグネチックスターラーつきヒーターで攪拌しながら80℃に加温した。それぞれのリードフレームをアクリル板に貼り付け、リードフレームがビーカーの開口部の中に入るようにふたをした。この間、硫化水素が発生してリードフレームに暴露させた。30分後ふたをはずし、リードフレームサンプルの反射濃度(BLK値)を微小面分光色差計(商品名:VSS400、日本電色工業株式会社製)を用い測定した。
個片化された表面実装型発光装置を60℃、湿度80%、硫化水素3ppmの環境下で96時間放置した。その後、該発光装置を取り出し、リードフレームの色変化(目視)および上記の手法で初期輝度を測定した。
図10に示す金型20において、第1凸部32の外周面32bを、第1凸部32の頂面32aに続く第1外周面と第1外周面に続く第2外周面とに分けた。第1外周面の頂面32aに対する傾斜角(頂面32aと第1外周面とがなす角の角度)を90°(実施例14および15)又は120°(実施例16)、第2外周面の頂面32に対する傾斜角(頂面32aと第2外周面の延長線とがなす角の角度)を140°(実施例14)又は150°(実施例15、16)とし、第1外周面と第2外周面との境界を、外周面32bにおける頂面32aから高さ100μm(実施例14、15)又は50μm(実施例16)の領域とした。なお、第1外周面と第2外周面とからなる外周面32bを有する第1凸部32と、底面32aに対する傾斜角が140°と一定である外周面32bを有する第1凸部32とを、縦横に交互に設けた。また、上側凹部33の底面33aの十点平均粗さRzを6.0μmに調整した。
第1凸部32の外周面32bを第1外周面と第2外周面とに分けず、頂面32aと外周面32bとがなす角の角度を150°(実施例17)又は140°(実施例18)とする以外は、実施例14と同様にして、MAP状リードフレーム付樹脂成形体を作製した。得られた樹脂成形体を上金型から脱型する際に、樹脂成形体の変形や界面剥離による破壊は発生しなかった。本実施例により、内壁面13bの底面13aに対する傾斜角が表9に示す値である凹部を有する樹脂成形体の集合体を得た。
1a,4a,4b,4c,4d 外側面
10,56a 第1リード
10a 第1インナーリード部、10b 第1アウターリード部
11,56b 第2リード
11a 第2インナーリード部、11b 第2アウターリード部
12,14,16,17,57 樹脂硬化体
12a 反射部、12b,17b 絶縁部、12c,17c 凹部開口面
13,15 凹部
13a 底部、13b 内壁面
18 めっき層
18a 最表面層、18b 第2金属層
20 金型
21 リードフレーム、22 フレーム単位、23 第1リード、24 第2リード
25 樹脂硬化体付リードフレーム
30 上金型、31 上側合わせ面、32 第1凸部、34 第2凸部
33 上側凹部、33a 底面
35 下金型、36 下側合わせ面
40 樹脂注入孔、41 プランジャー、42 ランナー、43 貫通孔
44 プランジャーポット、45 熱硬化性樹脂タブレットまたは液状の熱硬化性樹脂
50 表面実装型発光装置、51 発光素子
52a 第1金線、52b 第2金線
55 従来の樹脂成形体
58 樹脂バリ、59 樹脂欠け
60 第2斜面、61 第1斜面
Claims (20)
- 樹脂硬化体と複数のリードとが一体成形され、底部に前記複数のリードが露出する凹部を有する表面実装型発光装置用樹脂成形体であって、
前記凹部の開口面の十点平均粗さ(Rz)が1μm以上、10μm以下であり、
前記樹脂硬化体のガラス転移温度が10℃以上であり、前記ガラス転移温度が、熱機械分析装置(TMA)を用い、温度範囲-50~250℃、昇温速度5℃/分および試料サイズ長1~5mmの条件で測定された値であり、かつ、
前記凹部の開口面の460nmにおける光反射率が80%以上であり、前記樹脂成形体を180℃で72時間加熱した後の前記開口面における光反射率の保持率が90%以上である表面実装型発光装置用樹脂成形体。 - 前記樹脂硬化体の固体13C-核磁気共鳴スペクトルにおけるピークトップが、-1ppm~2ppmおよび13ppm~18ppmの範囲に少なくとも1つ存在する請求項1に記載の表面実装型発光装置用樹脂成形体。
- 前記樹脂硬化体が、(A)SiH基と反応性を有する炭素-炭素二重結合を1分子中に少なくとも2個含有する有機化合物、(B)1分子中に少なくとも2個のSiH基を含有する化合物、(C)ヒドロシリル化触媒、(D)SiH基と反応性を有する炭素-炭素二重結合を1分子中に少なくとも1個含有するシリコーン化合物、および(E)無機充填材を含有する熱硬化性樹脂組成物(X)の硬化物である請求項1または2に記載の表面実装型発光装置用樹脂成形体。
- 前記複数のリードの少なくとも1つがその表面に金属層を有し、前記金属層がその表面側に最表面層を有し、前記最表面層が厚み0.003~0.05μmのAu層、Au系合金層または光沢Ni層である請求項1~3のいずれか1項に記載の表面実装型発光装置用樹脂成形体。
- 前記金属層は、前記最表面層、および、前記リードの表面と前記最表面層との間に介在する第2金属層を有し、前記第2金属層は、Ag層、Pd層又はAg層とPd層との積層体である請求項4に記載の表面実装型発光装置用樹脂成形体。
- 前記金属層がめっき層である請求項4または5に記載の表面実装型発光装置用樹脂成形体。
- 前記凹部は、前記底部に露出する前記複数のリードの表面である底面を有し、
前記凹部の内壁面は、前記底面に連続して前記底面の周縁から立ち上がり、前記底面に対する傾斜角が45°~90°である第2斜面と、前記第2斜面に連続して前記第2斜面の周縁から前記開口面に向けて立ち上がり、前記底面に対する傾斜角が0°を超え45°以下である第1斜面と、を含み、前記第1斜面と前記第2斜面との境界が、前記内壁面における前記底面から高さ0μmを超え100μm以下の位置にある請求項1~6のいずれか1項に記載の表面実装型発光装置用樹脂成形体。 - 前記複数のリードは、互いに離隔するように配置される第1リードと第2リードとを含み、
前記樹脂硬化体は、前記第1リードと前記第2リードとの間に介在してこれらを絶縁する絶縁部を含み、前記絶縁部は、前記第1リードと前記第2リードとにより挟まれた状態で前記凹部の底部に露出する請求項1~7のいずれか1項に記載の表面実装型発光装置用樹脂成形体。 - 前記第1リードは、前記凹部の底部に露出する第1インナーリード部と、前記樹脂硬化体に接触する第1アウターリード部とを含み、かつ、前記第2リードは、前記凹部の底部に露出する第2インナーリード部と、前記樹脂硬化体に接触する第2アウターリード部とを含む請求項8に記載の表面実装型発光装置用樹脂成形体。
- 外側面に、前記第1アウターリード部および/または前記第2アウターリード部が露出する請求項9に記載の表面実装型発光装置用樹脂成形体。
- 前記外側面において、前記樹脂硬化体の露出面と、前記第1アウターリード部および/または前記第2アウターリード部の露出面とが、ほぼ同一平面上に存在する請求項10に記載の表面実装型発光装置用樹脂成形体。
- 前記第1インナーリード部および前記第2インナーリード部はその表面に前記金属層を有し、前記第1アウターリード部および前記第2アウターリード部はその表面に金属層を有していない請求項9~11のいずれか1項に記載の表面実装型発光装置用樹脂成形体。
- 前記複数のリードは、前記樹脂硬化体が充填されている切り欠き部を有する請求項1~12のいずれか1項に記載の表面実装型発光装置用樹脂成形体。
- 樹脂硬化体と複数のリードとが一体成形され、底部に前記複数のリードが露出する凹部を有し、前記樹脂硬化体における前記凹部の開口面の十点平均粗さ(Rz)が1μm以上、10μm以下である表面実装型発光装置用樹脂成形体の製造方法であって、
(1)前記樹脂硬化体の立体形状に対応する内部空間を有し、底面の十点平均粗さ(Rz)が0.5μm以上、15μm以下である上側凹部が所定位置に形成された上側合わせ面を有する上金型と、平坦な下側合わせ面を有する下金型と、樹脂注入孔と、を備える金型を用い、前記上側合わせ面と前記下側合わせ面とにより複数のリードを挟持して固定する工程と、
(2)前記金型内における前記上側凹部と前記複数のリードおよび/または前記下側合わせ面とにより形成される内部空間に、前記樹脂注入孔から液状の熱硬化性樹脂を注入する工程と、
(3)前記金型を所定の温度に加熱することにより、前記液状の熱硬化性樹脂を硬化させて、前記複数のリードの所定位置に前記熱硬化性樹脂の硬化物からなる樹脂硬化体が一体成形された前記樹脂成形体を作製する工程と、
(4)前記金型から前記樹脂成形体を脱型する工程と、
を含む表面実装型発光装置用樹脂成形体の製造方法。 - 前記複数のリードが、互いに離隔するように配置される、第1リードと第2リードとを含み、前記工程(2)において、前記第1リードと前記第2リードとの間の空間に液状の前記熱硬化性樹脂が注入される請求項14に記載の表面実装型発光装置用樹脂成形体の製造方法。
- 前記上側凹部が前記上側合わせ面の所定位置に形成された上金型と、平坦な前記下側合わせ面を有する前記下金型と、所定の間隔を空けて縦横に切り欠き部が形成された複数のリードと、を用いることにより、前記複数のリードの前記切り欠き部で囲まれた領域毎に前記樹脂硬化体を形成し、次いで前記切り欠き部に沿って前記複数のリードを切断することにより、複数個の前記樹脂成形体を得る請求項14または15に記載の表面実装型発光装置用樹脂成形体の製造方法。
- 前記複数のリードの少なくとも1つは表面に金属層を有している請求項16に記載の表面実装型発光装置用樹脂成形体の製造方法。
- 前記複数のリードの前記切り欠き部が、前記上側合わせ面の前記上側凹部が形成されていない領域と、前記下側合わせ面と、により挟持される請求項16または17に記載の表面実装型発光装置用樹脂成形体の製造方法。
- 請求項1~13のいずれか1項に記載の表面実装型発光装置用樹脂成形体と、前記樹脂成形体の凹部底部に実装され、複数のリードと通電可能に接続される発光素子と、前記発光素子を封止する透明樹脂層と、を備える表面実装型発光装置。
- 複数個の前記発光素子が実装される請求項19に記載の表面実装型発光装置。
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- 2012-09-26 WO PCT/JP2012/074757 patent/WO2013047606A1/ja active Application Filing
- 2012-09-26 US US14/344,075 patent/US9793456B2/en not_active Expired - Fee Related
- 2012-10-08 CN CN2012207558405U patent/CN203325962U/zh not_active Expired - Fee Related
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JP2016092153A (ja) * | 2014-10-31 | 2016-05-23 | Shマテリアル株式会社 | リードフレーム及びその製造方法 |
JP2018092974A (ja) * | 2016-11-30 | 2018-06-14 | 日亜化学工業株式会社 | パッケージ及びパッケージの製造方法、発光装置及び発光装置の製造方法 |
Also Published As
Publication number | Publication date |
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JPWO2013047606A1 (ja) | 2015-03-26 |
JP6164087B2 (ja) | 2017-07-19 |
CN203325962U (zh) | 2013-12-04 |
US20150008455A1 (en) | 2015-01-08 |
US9793456B2 (en) | 2017-10-17 |
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