JP2014008612A - Mold releasability imparting composition and method for manufacturing molded body - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a mold releasability imparting composition capable of effectively increase releasability when molding a molding material to obtain a molded body.SOLUTION: A mold releasability imparting composition 23 is used for imparting releasability on a surface of a metal mold 21 before molding a molding material 24 to obtain a molded body. The mold releasability imparting composition 23 includes: a thermosetting component; an inorganic filler; and a release agent. The release agent includes both fatty acid ester wax and oxidized or non-oxidized polyolefin wax.

Description

  The present invention relates to a mold releasability imparting composition used for imparting releasability to the surface of a mold before molding a molding material to obtain a molded body. Moreover, this invention relates to the manufacturing method of the molded object using this mold release property provision composition.

  A cured product of a thermosetting compound such as an epoxy compound, a polyester compound, a phenol compound, or a polyimide compound is excellent in adhesiveness, electrical characteristics, mechanical characteristics, heat resistance, chemical resistance, and the like. For this reason, the said thermosetting compound is used in field | areas, such as an adhesive agent, a laminated material, a mechanism component, a structural material, and a coating material. In particular, a molding material in which a filler is blended with an epoxy compound has good characteristics, so that a molding used for electronic parts, electrical equipment, office equipment, sealing materials, insulating materials, structural mechanism parts, etc. is obtained. Widely used in

  When a molding is obtained by molding the molding material, it is usually molded continuously under heat and pressure by a compression molding method, a transfer molding method or an injection molding method using a mold. When the molding material is continuously molded, the releasability of the molded body from the mold significantly affects the productivity. For this reason, a mold releasability imparting composition is used to impart releasability to the surface of the mold.

  As an example of the above-mentioned mold releasability imparting composition, the following Patent Document 1 includes (a) an epoxy resin, (b) a curing agent, (c) a curing accelerator, (d) a filler, (e) a release agent. A resin composition for mold surface release treatment containing a mold agent and (f) an antioxidant is disclosed. In the resin composition for mold surface release treatment, (e) a release agent component is 0.3 to 5% by weight with respect to the whole composition, and (f) an antioxidant component is 0 with respect to the whole composition. It is blended in the range of 3 to 5% by weight. In Patent Document 1, preferable release agents are montanic acid wax, montanic acid ester wax, partially saponified montanic acid ester wax, oxidized or nonoxidized polyethylene wax, oxidized or nonoxidized polypropylene wax, paraffin. It is described that it is at least one selected from the group consisting of system waxes and carnauba waxes.

  In the case of using the resin composition for mold surface release treatment described in Patent Document 1, the resin composition for mold surface release treatment is dummy-molded before molding of the molding material. By this dummy molding, mold release properties are imparted to the surface of the mold. Next, a molding material is obtained by molding a molding material using a mold provided with releasability.

  In addition, when an optical semiconductor element (for example, an LED), which is a light emitting element used in an optical semiconductor device, is in direct contact with the atmosphere, the light emission characteristics of the optical semiconductor element rapidly deteriorate due to moisture in the atmosphere or floating dust. . For this reason, the said optical semiconductor element is normally sealed with the sealing compound for optical semiconductor devices. In order to fill the sealant, a molded body having a frame portion is disposed on a lead frame on which the optical semiconductor element is mounted. The sealing agent is filled inside the molded body having the frame portion. The said molded object may be called a reflector, a case material, or a housing. An optical semiconductor device including such a molded body is disclosed in, for example, Patent Document 2 below.

Japanese Patent Application Laid-Open No. 07-309998 JP 2006-156704 A

  In Patent Document 1, only a number of mold release agents are listed regarding the mold release agent. In the examples, only one type of polyethylene wax or only one type of montanic acid ester is used. Absent.

  Even when a release agent as described in Patent Document 1 is used, the mold release property of the mold surface may not be sufficiently high.

  Patent Document 1 only describes an example in which an epoxy resin-based sealant for semiconductor sealing is molded to form a sealant for sealing a semiconductor element. When molding the sealant, the mold releasability is required to be somewhat high, but from the shape of the sealant and because the contact area between the sealant and the mold is relatively small, Even if the mold releasability is not very high, the sealant can be molded well.

  On the other hand, in the case of forming a molded body having a frame portion and filled with a sealant in the frame portion, a conventional method for manufacturing a molded body is a metal as described in Patent Document 1. No mold releasability imparting composition is used. In a conventional method for producing a molded body, it may be difficult to form a molded body having the frame portion satisfactorily. Moreover, in the conventional manufacturing method of a molded object, since the contact area of the molded object which has the said frame part, and a metal mold | die is comparatively large, it is difficult to shape | mold a molded object which has the said frame part favorably. In particular, when a large number of molded articles having a frame portion are to be molded continuously, the molding may be impossible at an early stage.

  Further, when a molded body having a frame portion is obtained by a conventional method of manufacturing a molded body, and then an optical semiconductor device is manufactured using the molded body, the optical semiconductor device is kept under high temperature or high humidity. When exposed, the sealant may peel from the molded body having the frame portion. Furthermore, when the optical semiconductor device is used while being energized at high temperature and high humidity, the brightness of light extracted from the optical semiconductor device may be reduced.

  An object of the present invention is to provide a mold releasability imparting composition capable of effectively enhancing mold releasability when molding a molding material to obtain a molded product, and the mold releasability imparting composition. It is providing the manufacturing method of the used molded object.

  A limited object of the present invention is to obtain an optical semiconductor device having a frame part and having a molded body filled with a sealing agent in the frame part, and the optical semiconductor device is at a high temperature or high temperature. Mold releasability imparting composition capable of suppressing delamination from molded article having sealing agent frame even when exposed to moisture, and molded article using the mold releasability imparting composition It is to provide a manufacturing method.

  A limited object of the present invention is to obtain an optical semiconductor device having a frame portion and having a molded body filled with a sealing agent in the frame portion, and the optical semiconductor device is subjected to high temperature and high humidity. By providing a mold releasability-imparting composition that can make it difficult to lower the luminous intensity even if it is used by energizing with, and a method for producing a molded body using the mold releasability-imparting composition is there.

  According to a wide aspect of the present invention, there is provided a mold releasability imparting composition used for imparting releasability to the surface of a mold before molding a molding material to obtain a molded body, A mold releasability imparting composition comprising a curable component, an inorganic filler, and a release agent, wherein the release agent contains both a fatty acid ester wax and an oxidized or non-oxidized polyolefin wax. Things are provided.

  In 100% by weight of the mold releasability imparting composition according to the present invention, the content of the fatty acid ester wax is 0.5% by weight to 3% by weight, and the oxidized or non-oxidized polyolefin wax The content is preferably 1% by weight or more and 9% by weight or less.

  The inorganic filler is preferably silica. It is preferable that the inorganic filler contains both a spherical filler and a crushed filler. It is preferable that the thermosetting component contains an epoxy compound and a curing agent. It is preferable that the thermosetting component contains a curing accelerator. It is preferable that the thermosetting component contains both a bisphenol A type epoxy compound and a novolac type epoxy compound.

  In a specific aspect of the mold releasability imparting composition according to the present invention, the mold releasability imparting composition is used before forming a molding material by molding a molding material by transfer molding.

  In a specific aspect of the mold releasability imparting composition according to the present invention, the mold releasability imparting composition is a molded part having a frame portion disposed on the side of an optical semiconductor element in an optical semiconductor device. Used before getting the body.

  In a specific aspect of the mold releasability imparting composition according to the present invention, the mold releasability imparting composition is used before a white molding material is obtained by molding a white molding material.

  According to a wide aspect of the present invention, a mold release property is imparted to the surface of a mold using the mold release property-imparting composition described above, and then a molding material is molded to obtain a molded article. A manufacturing method is provided.

  On the specific situation with the manufacturing method of the molded object which concerns on this invention, the said molding material is shape | molded by transfer molding and a molded object is obtained.

  On the specific situation with the manufacturing method of the molded object which concerns on this invention, in an optical semiconductor device, the molded object which has a frame part arrange | positioned at the side of an optical semiconductor element is obtained.

  In a specific aspect of the method for producing a molded body according to the present invention, a white molded body is obtained by molding a white molding material.

  The mold releasability imparting composition according to the present invention includes a thermosetting component, an inorganic filler, and a release agent, and the release agent comprises a fatty acid ester wax and an oxidized or non-oxidized polyolefin wax. Since both are contained, the mold release property can be effectively enhanced when the molding material is molded to obtain a molded body.

1 (a) to 1 (e) show molding using a mold releasability imparting composition according to an embodiment of the present invention, imparting releasability to a mold surface, and molding a molding material. It is typical sectional drawing for demonstrating an example of each process of obtaining a body. 2 (a) and 2 (b) schematically illustrate an example of an optical semiconductor device including a molded body obtained by molding a molding material using a mold release property imparting composition according to an embodiment of the present invention. It is sectional drawing and a perspective view shown in figure. FIG. 3 is a cross-sectional view schematically showing a modification of the optical semiconductor device shown in FIG.

  Hereinafter, the present invention will be described in detail.

  The mold releasability imparting composition according to the present invention is used to impart releasability to the surface of a mold before molding a molding material to obtain a molded product. The mold releasability imparting composition according to the present invention includes a thermosetting component (A), an inorganic filler (B), and a release agent (C). The mold release agent (C) contains both a fatty acid ester wax (C1) and an oxidized or non-oxidized polyolefin wax (C2).

  By adopting the above-described composition in the mold releasability imparting composition according to the present invention, the releasability can be effectively enhanced when a molding material is molded to obtain a molded body. Moreover, a molded object can be easily peeled and taken out from the surface of the mold, and the continuous moldability can be improved. Furthermore, the shape of the molded body taken out from the mold can be improved. For example, the occurrence of chipping at the corners of the molded body can be suppressed.

  Further, by adopting the above-described composition in the mold releasability imparting composition according to the present invention, the mold releasability imparting composition according to the present invention is used to impart releasability to the surface of the mold. In addition, when an optical semiconductor device having a frame portion and having a molded body filled with a sealing agent in the frame portion is obtained, even if the optical semiconductor device is exposed to high temperature or high humidity, It becomes difficult for the sealant to peel from the molded body having the frame portion.

  Further, by adopting the above-described composition in the mold releasability imparting composition according to the present invention, the mold releasability imparting composition according to the present invention is used to impart releasability to the surface of the mold. In addition, when an optical semiconductor device having a frame portion and having a molded body in which the sealant is filled in the frame portion is obtained, the optical semiconductor device may be used while being energized at high temperature and high humidity. , The light intensity is difficult to decrease.

(Details of mold releasability imparting composition and molding material)
The mold releasability imparting composition includes a thermosetting component (A), an inorganic filler (B), and a release agent (C). The release agent (C) contained in the mold releasability imparting composition contains both a fatty acid ester wax (C1) and an oxidized or non-oxidized polyolefin wax (C2). The molding material preferably contains a thermosetting component (A). The molding material preferably contains an inorganic filler (B). The inorganic filler (B) contained in the molding material is preferably a white inorganic filler, and more preferably titanium oxide.

  The thermosetting component (A) contained in the mold releasability imparting composition and the thermosetting component (A) contained in the molding material may be the same or different. The inorganic filler (B) contained in the mold releasability imparting composition and the inorganic filler (B) contained in the molding material may be the same or different.

  Hereinafter, each component used for the said mold release property provision composition and the said molding material is demonstrated concretely.

[Thermosetting component (A)]
The mold releasability imparting composition contains a thermosetting component (A). The molding material preferably contains a thermosetting component (A). The thermosetting component (A) can be cured by applying heat. The thermosetting component (A) preferably contains a thermosetting compound (A1) and a curing agent (A2). In order to further enhance the thermosetting property, the thermosetting component (A) preferably contains a curing accelerator (A3).

  As said thermosetting compound (A1), an epoxy compound, a silicone compound, a polyester compound, a phenol compound, a polyimide compound, etc. are mentioned. As for the said thermosetting compound (A1), only 1 type may be used and 2 or more types may be used together.

  The thermosetting compound (A1) contained in the mold releasability imparting composition is preferably an epoxy compound. The thermosetting compound (A1) contained in the molding material is preferably an epoxy compound or a silicone compound, and is preferably an epoxy compound. The thermosetting compound (A1) contained in the molding material is preferably an epoxy compound or a silicone compound having two or more epoxy groups, and is preferably an epoxy compound having two or more epoxy groups. As for the said epoxy compound, only 1 type may be used and 2 or more types may be used together.

  The epoxy compound has an epoxy group. By using the epoxy compound as the thermosetting compound (A1) contained in the mold releasability imparting composition, the mold releasability imparting composition can be easily molded.

  Specific examples of the epoxy compound include a bisphenol type epoxy compound, a novolac type epoxy compound, a glycidyl ester type epoxy compound obtained by reacting a polychloric acid compound and epichlorohydrin, a polyamine compound and epichlorohydrin. Glycidylamine type epoxy compounds, glycidyl ether type epoxy compounds, aliphatic epoxy compounds, hydrogenated aromatic epoxy compounds, epoxy compounds having an alicyclic skeleton, and heterocyclic epoxy compounds such as triglycidyl isocyanurate obtained by reaction Etc. Examples of the polychloric acid compound include phthalic acid and dimer acid. Examples of the polyamine compound include diaminodiphenylmethane and isocyanuric acid. Examples of the novolac type epoxy compound include a phenol novolac type epoxy compound and a cresol novolac type epoxy compound.

  From the viewpoint of further improving mold release properties and further improving continuous moldability when molding a molding material to obtain a molded body, the thermosetting component (A) and the epoxy compound are each bisphenol A. It is preferable to contain at least one of a type epoxy compound and a novolac type epoxy compound, more preferably a bisphenol A type epoxy compound, and more preferably a novolac type epoxy compound. The epoxy compound preferably has a bisphenol skeleton or a novolak skeleton. When the molding material is molded to obtain a molded body, the thermosetting component (A) and the epoxy compound are each bisphenol A from the viewpoint of further improving the mold release property and further improving the continuous moldability. It is preferable to contain both a type epoxy compound and a novolac type epoxy compound.

  The novolac epoxy compound is preferably a phenol novolac epoxy compound or a cresol novolac epoxy compound.

  The thermosetting functional group equivalent of the thermosetting compound (A1) is preferably 100 or more, and preferably 3000 or less. When the thermosetting functional group equivalent is 100 or more, the mold releasability imparting composition and the moldability of the molding material are further improved. The intensity | strength of a molded object becomes it still higher that the said thermosetting functional group equivalent is 3000 or less. When the thermosetting compound (A1) is the epoxy compound, the thermosetting functional group equivalent means an epoxy equivalent.

  The compounding quantity of the said thermosetting compound (A1) and the said epoxy compound is suitably adjusted so that it may harden | cure moderately by provision of heat, and is not specifically limited.

  The content of the thermosetting compound (A1) and the epoxy compound in 100% by weight of the mold releasability imparting composition is preferably 3% by weight or more, more preferably 5% by weight or more, and still more preferably. It is 10% by weight or more, preferably 99% by weight or less, more preferably 95% by weight or less, and still more preferably 80% by weight or less. When the contents of the thermosetting compound (A1) and the epoxy compound are equal to or higher than the lower limit, the mold releasability imparting composition is more effectively cured by heating. The heat resistance of a molded object becomes it still higher that content of the said thermosetting compound (A1) and the said epoxy compound is below the said upper limit.

  The content of the thermosetting compound (A1) and the epoxy compound or the silicone compound is preferably 3% by weight or more, more preferably 5% by weight or more, and still more preferably 10% by weight in 100% by weight of the molding material. % Or more, preferably 99% by weight or less, more preferably 95% by weight or less, and still more preferably 80% by weight or less. When the content of the thermosetting compound (A1) and the epoxy compound is not less than the lower limit, the molding material is more effectively cured by heating. The heat resistance of a molded object becomes it still higher that content of the said thermosetting compound (A1) and the said epoxy compound is below the said upper limit.

  In the case of using a bisphenol A type epoxy compound and a novolac type epoxy compound in combination, in the mold release property-imparting composition and the molding material, the content of the bisphenol A type epoxy compound with respect to the content of the novolac type epoxy compound The weight ratio (bisphenol A type epoxy compound / novolak type epoxy compound) is preferably 0.01 or more and 100 or less, more preferably 0.03 or more and 30 or less, and more preferably 0.07 or more and 15 or less. More preferably. The content of the bisphenol A type epoxy compound and the content of the novolak type epoxy compound indicate the content in 100% by weight of the mold releasability imparting composition and 100% by weight of the molding material. That is, the mold releasability imparting composition and the molding material are each in a weight ratio of bisphenol A type epoxy compound and novolac type epoxy compound (bisphenol A type epoxy compound: novolak type epoxy compound), from 1: 100 to It is preferably included at 100: 1, more preferably at 1:30 to 30: 1, and still more preferably at 1:15 to 15: 1.

  The thermosetting component (A) contained in the mold releasability imparting composition and the molding material contains the curing agent (A2) so that it can be efficiently cured by application of heat. Is preferred. The curing agent (A2) includes a curing catalyst for curing the silicone compound. Further, when the curing agent (A2) is a silicone compound, the curing agent (A2) is not necessarily used. The curing agent (A2) cures the thermosetting compound (A1). As said hardening | curing agent (A2), the well-known hardening | curing agent used as a hardening | curing agent of a thermosetting compound can be used. As for the said hardening | curing agent (A2), only 1 type may be used and 2 or more types may be used together.

  As the curing agent (A2), triphenylphosphine is formed by a shell formed of an acid anhydride, dicyandiamide, a phenol compound, a hydrazide compound, an imidazole compound, a compound having a triazine ring, a methyl (meth) acrylate resin, a styrene resin, or the like. A latent curing agent (for example, “EPCAT-P” and “EPCAT-PS” manufactured by Nippon Kayaku Co., Ltd.), a polyurea polymer or a radical polymer formed by a shell formed with a (curing agent) is coated with an amine. A latent curing agent coated with a curing agent such as, a curing agent such as modified imidazole dispersed in an epoxy resin, confined and pulverized (“Novacure” manufactured by Asahi Kasei E-Materials) HXA3792 "and" HXA3932HP "), in thermoplastic polymers A latent curing agent in which a curing agent is dispersed and contained, and an imidazole latent curing agent coated with a tetrakisphenol compound (for example, “TEP-2E4MZ” and “HIPA-2E4MZ” manufactured by Nippon Soda Co., Ltd.) Can be mentioned. A curing agent (A2) other than these may be used. Especially, an acid anhydride or a phenol compound is preferable, and a phenol compound is more preferable. The curing agent (A2) is preferably an acid anhydride curing agent or a phenol curing agent, and more preferably a phenol curing agent.

  From the viewpoint of further improving the adhesion with a member such as a sealant and a lead frame in contact with the molded body, the curing agent (A2) contained in the molding material is an acid anhydride curing agent. Is more preferable. The thermosetting component (A) contained in the molding material preferably contains an acid anhydride curing agent. By using an acid anhydride curing agent, it is possible to maintain high curability and further suppress molding unevenness of the molded body. The mold releasability imparting composition is a molding in which the epoxy compound contained in the molding material has two or more epoxy groups, and an epoxy compound having two or more epoxy groups and an acid anhydride curing agent. It is preferably used before molding the material.

  As the acid anhydride curing agent, any of an acid anhydride having an aromatic skeleton and an acid anhydride having an alicyclic skeleton can be used.

  Preferred examples of the acid anhydride curing agent include phthalic anhydride, maleic anhydride, trimellitic anhydride, pyromellitic anhydride, hexahydrophthalic anhydride, tetrahydrophthalic anhydride, methyl nadic anhydride, nadic anhydride, glutaric anhydride. And methylhexahydrophthalic anhydride and methyltetrahydrophthalic anhydride.

  The acid anhydride curing agent preferably does not have a double bond. Preferable acid anhydride curing agents having no double bond include hexahydrophthalic anhydride and methylhexahydrophthalic anhydride.

  The compounding ratio of the thermosetting compound (A1) and the curing agent (A2) is not particularly limited. The content of the curing agent (A2) is preferably 0.5 parts by weight or more, more preferably 1 part by weight or more, further preferably 2 parts by weight or more with respect to 100 parts by weight of the thermosetting compound (A1). The amount is particularly preferably 3 parts by weight or more, preferably 500 parts by weight or less, more preferably 300 parts by weight or less, and still more preferably 100 parts by weight or less.

  Moreover, in the said mold release property provision composition and the said molding material, the equivalent of the thermosetting functional group equivalent of the whole said thermosetting compound (A1), and the hardening | curing agent equivalent of the said whole hardening | curing agent (A2). The ratio (thermosetting functional group equivalent: curing agent equivalent) is preferably 0.3: 1 to 2: 1, and more preferably 0.5: 1 to 1.5: 1.

  In order to accelerate the reaction between the thermosetting compound (A1) and the curing agent (A2), the thermosetting component (A) contained in the mold release property-imparting composition is a curing accelerator ( A3) is preferably contained, and the thermosetting component (A) contained in the molding material preferably contains a curing accelerator (A3). By using the curing accelerator (A3), the mold releasability imparting composition and the molding material are further improved in curability, and further, the heat resistance of the molded body is further enhanced. As for the said hardening accelerator (A3), only 1 type may be used and 2 or more types may be used together.

  It is preferable that the said hardening accelerator (A3) contained in the said molding material contains the hardening accelerator which has basicity. By using a curing accelerator having basicity, the curability of the molding material is further improved.

  Whether the curing accelerator (A3) has basicity is determined by putting 1 g of the curing accelerator in 10 g of a liquid containing 5 g of acetone and 5 g of pure water, and heating with stirring at 80 ° C. for 1 hour. Next, when an insoluble component in the liquid after heating is removed by filtration to obtain an extract, it is judged that the pH of the extract is basic.

  Examples of the curing accelerator (A3) include urea compounds, onium salt compounds, imidazole compounds, phosphorus compounds, amine compounds, and organometallic compounds.

  Examples of the urea compound include urea, aliphatic urea compounds, and aromatic urea compounds. Specific examples of the urea compound include urea, methylurea, 1,1-dimethylurea, 1,3-dimethylurea, 1,1,3,3-tetramethylurea, 1,3-diphenylurea, and tri-n-. Examples include butylthiourea. Urea compounds other than these may be used.

  Examples of the onium salt compounds include ammonium salts, phosphonium salts, and sulfonium salt compounds.

  Examples of the imidazole compound include 2-undecylimidazole, 2-heptadecylimidazole, 2-methylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2-phenyl-4-methylimidazole, 1-benzyl- 2-methylimidazole, 1-benzyl-2-phenylimidazole, 1,2-dimethylimidazole, 1-cyanoethyl-2-methylimidazole, 1-cyanoethyl-2-ethyl-4-methylimidazole, 1-cyanoethyl-2-un Decylimidazole, 1-cyanoethyl-2-phenylimidazole, 1-cyanoethyl-2-undecylimidazolium trimellitate, 1-cyanoethyl-2-phenylimidazolium trimellitate, 2,4-diamino-6- [2 ′ -Methyl Midazolyl- (1 ′)]-ethyl-s-triazine, 2,4-diamino-6- [2′-undecylimidazolyl- (1 ′)]-ethyl-s-triazine, 2,4-diamino-6 [2′-Ethyl-4′-methylimidazolyl- (1 ′)]-ethyl-s-triazine, 2,4-diamino-6- [2′-methylimidazolyl- (1 ′)]-ethyl-s-triazine Isocyanuric acid adduct, 2-phenylimidazole isocyanuric acid adduct, 2-methylimidazole isocyanuric acid adduct, 2-phenyl-4,5-dihydroxymethylimidazole and 2-phenyl-4-methyl-5-dihydroxymethylimidazole Can be mentioned.

  The phosphorus compound contains phosphorus and is a phosphorus-containing compound. Examples of the phosphorus compound include triphenylphosphine, tetraphenylphosphonium tetraphenylborate, tetra-n-butylphosphonium-o, o-diethylphosphorodithioate, tetra-n-butylphosphonium-tetrafluoroborate, and tetra-n-. Examples thereof include butylphosphonium-tetraphenylborate. Phosphorus compounds other than these may be used.

  Examples of the amine compound include diethylamine, triethylamine, diethylenetetramine, triethylenetetramine, 4,4-dimethylaminopyridine, diazabicycloalkane, diazabicycloalkene, quaternary ammonium salt, triethylenediamine, and tri-2,4. , 6-dimethylaminomethylphenol. You may use the salt of these compounds. Phenylphosphine, tetraphenylphosphonium tetraphenylborate, tetra-n-butylphosphonium-o, o-diethylphosphorodithioate, tetra-n-butylphosphonium-tetrafluoroborate, tetra-n-butylphosphonium-tetraphenylborate It is done.

  Examples of the organometallic compound include alkali metal compounds and alkaline earth metal compounds. Specific examples of the organometallic compound include zinc naphthenate, cobalt naphthenate, tin octylate, cobalt octylate, bisacetylacetonate cobalt (II), and trisacetylacetonate cobalt (III).

  From the viewpoint of further enhancing the curability of the mold releasability imparting composition and the molding material, the curing accelerator (A3) is preferably a urea compound, an onium salt compound or a phosphorus compound. The curing accelerator (A3) is preferably a urea compound, preferably an onium salt compound, and preferably a phosphorus compound.

  The compounding ratio of the thermosetting compound (A1) and the curing accelerator (A3) is not particularly limited. The content of the curing accelerator (A3) is preferably 0.01 parts by weight or more, more preferably 0.1 parts by weight or more, preferably 100 parts by weight with respect to 100 parts by weight of the thermosetting compound (A1). Parts or less, more preferably 10 parts by weight or less, still more preferably 5 parts by weight or less.

  The content of the basic curing accelerator is preferably 0.01 parts by weight or more, more preferably 0.1 parts by weight or more, preferably 100 parts by weight based on 100 parts by weight of the thermosetting compound (A1). The amount is not more than parts by weight, more preferably not more than 10 parts by weight, still more preferably not more than 5 parts by weight. When the content of the curing accelerator having basicity is not less than the above lower limit and not more than the above upper limit, the curability of the curable composition is further increased, and the molding unevenness of the molded body is more unlikely to occur.

[Inorganic filler (B)]
The mold releasability imparting composition contains an inorganic filler (B). The molding material preferably contains an inorganic filler (B). As for the said inorganic filler (B), only 1 type may be used and 2 or more types may be used together.

  Specific examples of the inorganic filler (B) include silica, alumina, mica, beryllia, potassium titanate, barium titanate, strontium titanate, calcium titanate, zirconium oxide, antimony oxide, aluminum borate, and aluminum hydroxide. , Magnesium oxide, calcium carbonate, magnesium carbonate, aluminum carbonate, calcium silicate, aluminum silicate, magnesium silicate, calcium phosphate, calcium sulfate, barium sulfate, silicon nitride, boron nitride, clays such as calcined clay, talc and silicon carbide Is mentioned.

  From the viewpoint of further improving the moldability of the mold releasability imparting composition and the molding material, the inorganic filler (B) is preferably silica. Furthermore, when the optical semiconductor device is exposed to high temperature or high humidity, it is difficult to peel off the sealing agent from the molded body, and from the viewpoint of further improving the reflow resistance, the above mold release property imparting composition The inorganic filler (B) contained in the product and the molding material is preferably silica. The inorganic filler (B) contained in the molding material preferably contains silica. Since silica has a low linear expansion coefficient, the reflow resistance of the molded product is further enhanced by using silica.

  From the viewpoint of further increasing the reflectance of the molded body, the inorganic filler (B) contained in the molding material preferably contains a white inorganic filler, and more preferably contains titanium oxide. . By using a white inorganic filler, a molded article having high light reflectance can be obtained. By using the titanium oxide, it is possible to obtain a molded article having a high light reflectance as compared with a case where only a filler different from titanium oxide is used.

  Examples of the white inorganic filler include titanium oxide, zirconium oxide, aluminum oxide, zinc oxide, and barium sulfate.

  The titanium oxide is preferably rutile titanium oxide or anatase titanium oxide. By using rutile-type titanium oxide, a molded article having further excellent heat resistance can be obtained, and the quality is hardly lowered even when the optical semiconductor device is used in a harsh environment. The anatase type titanium oxide has a lower hardness than the rutile type titanium oxide. For this reason, the moldability of the said curable composition becomes still higher by use of anatase type titanium oxide.

  The titanium oxide preferably includes rutile type titanium oxide surface-treated with aluminum oxide. In 100% by weight of the inorganic filler (B) contained in the molding material, the content of rutile titanium oxide surface-treated from the aluminum oxide is preferably 10% by weight or more, more preferably 30% by weight or more. 100% by weight or less. The total amount of the titanium oxide may be rutile titanium oxide surface-treated with the aluminum oxide. Use of the rutile type titanium oxide surface-treated with the aluminum oxide further increases the heat resistance of the molded body.

  Examples of the rutile-type titanium oxide surface-treated with the aluminum oxide include, for example, a product number manufactured by Ishihara Sangyo Co., Ltd., which is rutile chlorine method titanium oxide, and a product number manufactured by Ishihara Sangyo Co., Ltd., which is rutile sulfuric acid method titanium oxide. : R-630 and the like.

  The inorganic filler (B) preferably includes a spherical filler (B1). The inorganic filler (B) preferably includes a crushed filler (B2). The inorganic filler (B) preferably includes both the spherical filler (B1) and the crushed filler (B2). Moreover, the moldability of the said mold release property provision composition and the said molding material becomes still higher by combined use with the said spherical filler (B1) and the said crushing filler (B2). The spherical filler (B1) is preferably spherical silica. The crushed filler (B2) is preferably crushed silica.

  The spherical filler (B1) is spherical. The spherical filler (B1) refers to a filler having an aspect ratio of 2 or less. The spherical filler (B1) may be a true sphere, an elliptical sphere obtained by flattening a sphere, or a shape similar to these.

  The crushed filler (B2) is a crushed filler. The aspect ratio of the crushed filler (B2) is not particularly limited. The aspect ratio of the crushed filler (B2) is preferably 1.5 or more, and preferably 20 or less. A crushing filler having an aspect ratio of less than 1.5 is relatively expensive. Accordingly, the cost of the mold releasability imparting composition is increased. When the aspect ratio is 20 or less, the crushing filler (B2) can be easily filled.

  The aspect ratio of the crushing filler (B2) is measured, for example, by using a digital image analysis type particle size distribution measuring device (trade name: FPA, manufactured by Nippon Luft Co., Ltd.). Can be obtained.

  Preferred examples of the spherical filler (B1) include silica, alumina, potassium titanate, zirconium oxide, strontium titanate, aluminum borate, magnesium oxide, calcium carbonate, magnesium carbonate, calcium silicate, magnesium silicate, calcium phosphate and Examples thereof include calcium sulfate. As for the said spherical filler (B1), only 1 type may be used and 2 or more types may be used together.

  Preferred examples of the crushed filler (B2) include silica, antimony oxide, zirconium oxide, aluminum hydroxide, magnesium hydroxide, barium sulfate, magnesium carbonate, barium carbonate, alumina, mica, beryllia, barium titanate, titanate. Potassium, strontium titanate, calcium titanate, aluminum carbonate, aluminum silicate, calcium carbonate, calcium silicate, magnesium silicate, silicon nitride, boron nitride, calcined clay, etc., talc, aluminum borate, silicon carbide, etc. Can be mentioned. As for the said crushing filler (B2), only 1 type may be used and 2 or more types may be used together.

  From the viewpoint of improving the moldability and obtaining a molded body excellent in thermal conductivity and light reflection characteristics, the crushed filler (B2) is composed of silica, alumina, magnesium oxide, antimony oxide, zirconium oxide, aluminum hydroxide or Magnesium hydroxide is preferred.

  The average particle size of the inorganic filler (B), the average particle size of the spherical filler (B1), and the average particle size of the crushed filler (B2) are each preferably 0.1 μm or more, preferably 100 μm or less. is there. When the average particle size is not less than the above lower limit, the mold releasability imparting composition and the moldability of the molding material are further improved. When the average particle size is less than or equal to the above upper limit, the appearance defect of the molded body is more difficult to occur.

  The average particle diameter in the inorganic filler (B), the average particle diameter in the spherical filler (B1), and the average particle diameter in the crushed filler (B2) are 50% integrated value in the volume-based particle size distribution curve. Is the particle size value at the time. The average particle size can be measured using, for example, a laser beam type particle size distribution meter. As a commercial product of the laser beam type particle size distribution analyzer, “LS 13 320” manufactured by Beckman Coulter, Inc. can be cited.

  In 100% by weight of the mold releasability imparting composition and 100% by weight of the molding material, the content of the inorganic filler (B) is preferably 5% by weight or more, more preferably 10% by weight or more. Preferably it is 20 weight% or more, Preferably it is 95 weight% or less, More preferably, it is 90 weight% or less, More preferably, it is 85 weight% or less. When the content of the inorganic filler (B) is not less than the above lower limit and not more than the above upper limit, the mold releasability imparting composition and the moldability of the molding material are further enhanced.

  When the spherical filler (B1) and the crushed filler (B2) are used in combination, in the mold releasability imparting composition and the molding material, the content of the spherical filler (B1) is the above. The weight ratio to the content of the crushed filler (B2) (spherical filler (B1) / crushed filler (B2)) is preferably 0.03 or more and 30 or less, and is 0.07 or more and 15 or less. More preferably. Content of the said spherical filler (B1) and content of the said crushing filler (B2) show content in 100 weight% of the said mold release property provision composition and 100 weight% of the said molding materials. . That is, the mold releasability imparting composition and the molding material are respectively in a weight ratio of the spherical filler (B1) and the crushed filler (B2) (spherical filler (B1): crushed filler (B2). )), It is preferably included at 1:30 to 30: 1, and more preferably at 1:15 to 15: 1. When the weight ratio (spherical filler (B1): crushed filler (B2)) is satisfied, the mold releasability imparting composition and the moldability of the molding material are further enhanced. Further, when the content of the spherical filler (B1) is relatively increased, the molded body is less likely to be brittle, the processability of the molded body is further enhanced, and cracks and chips are less likely to occur in the molded body. . When the content of the crushed filler (B2) is relatively increased, the strength of the molded body is further increased.

[Release agent (C)]
The mold releasability imparting composition contains a release agent (C). The release agent (C) contains both the fatty acid ester wax (C1) and the oxidized or non-oxidized polyolefin wax (C2). The combined use of this specific mold release agent (C) greatly contributes to enhancing mold release properties when a molding material is molded to obtain a molded body.

  In JP-A-07-309998 described above, preferable release agents are montanic acid wax, montanic acid ester wax, partially saponified montanic acid ester wax, oxidized or non-oxidized polyethylene wax, oxidized or non-oxidized It is described that it is at least one selected from the group consisting of oxidized polypropylene wax, paraffin wax and carnauba wax. However, here, regarding the release agent, only a number of release agents are listed, and in the examples, only one type of polyethylene wax or only one type of montanic acid ester is used. Absent. Here, there is no description regarding selecting a configuration in which two types of fatty acid ester wax (C1) and oxidized or non-oxidized polyolefin wax (C2) are used in combination. Compared to the case where only one fatty acid ester wax (C1) is used or only one kind of oxidized or non-oxidized polyolefin wax (C2) is used, the fatty acid ester wax (C1) is oxidized or non-oxidized. When both the polyolefin wax (C2) is used, the releasability can be sufficiently enhanced, and the continuous moldability can be effectively enhanced.

  Specific examples of the fatty acid ester wax (C1) include saturated or unsaturated fatty acid glycerin ester, polyglycerin ester or sorbitol ester. Examples of monovalent saturated or unsaturated fatty acids include capric acid, lauric acid, myristic acid, pentadecylic acid, palmitic acid, stearic acid, arachidic acid, behenic acid, and montanic acid. Examples of the divalent saturated or unsaturated fatty acid include oleic acid, linoleic acid, linolenic acid, arachidonic acid and erucic acid.

  Specific examples of the oxidized or non-oxidized polyolefin wax (C2) include oxidized or non-oxidized polyethylene wax, oxidized or non-oxidized polypropylene wax and oxidized or non-oxidized olefin copolymer wax. Examples of the oxidized or non-oxidized olefin copolymer wax include oxidized or non-oxidized ethylene copolymer wax and oxidized or non-oxidized polypropylene wax.

  In 100% by weight of the mold releasability imparting composition, the content of the fatty acid ester wax (C1) is preferably 0.01% by weight or more, more preferably 0.1% by weight or more, and still more preferably 0.8%. It is 5% by weight or more, preferably 20% by weight or less, more preferably 10% by weight or less, and further preferably 3% by weight or less. When the content of the fatty acid ester wax (C1) is not less than the above lower limit and not more than the above upper limit, the mold releasability is further enhanced when the molding material is molded to obtain a molded body.

  The content of the oxidized or non-oxidized polyolefin wax (C2) is preferably 0.01% by weight or more, more preferably 0.1% by weight or more, and still more preferably in 100% by weight of the mold releasability imparting composition. Is 1% by weight or more, preferably 30% by weight or less, more preferably 20% by weight or less, and still more preferably 9% by weight or less. When the content of the oxidized or non-oxidized polyolefin wax (C2) is not less than the above lower limit and not more than the above upper limit, the releasability is further enhanced when the molding material is molded to obtain a molded body.

  In 100% by weight of the mold releasability imparting composition, the content of the fatty acid ester wax (C1) is preferably 0.5% by weight or more and 3% by weight or less. The content of the wax (C2) is preferably 1% by weight or more and 9% by weight or less, the content of the fatty acid ester wax (C1) is 0.5% by weight or more and 3% by weight or less, and The content of the oxidized or non-oxidized polyolefin wax (C2) is more preferably 1 wt% or more and 9 wt% or less.

  The total content of the fatty acid ester wax (C1) and the oxidized or non-oxidized polyolefin wax (C2) in 100% by weight of the mold releasability imparting composition is preferably 0.02% by weight or more. More preferably 0.2% by weight or more, further preferably 1.5% by weight or more, preferably 40% by weight or less, more preferably 30% by weight or less, still more preferably 20% by weight or less, particularly preferably 12% by weight. It is as follows. When the total content of the fatty acid ester wax (C1) and the oxidized or non-oxidized polyolefin wax (C2) is not less than the lower limit and not more than the upper limit, a molding material is molded to obtain a molded body. , The releasability is further enhanced.

[Antioxidant (D)]
The mold releasability imparting composition preferably contains an antioxidant (D). The molding material preferably contains an antioxidant (D). As said antioxidant (D), a phenolic antioxidant, phosphorus antioxidant, an amine antioxidant, etc. are mentioned. As for the said antioxidant (D), only 1 type may be used and 2 or more types may be used together.

  Examples of commercially available phenolic antioxidants include IRGANOX 1010, IRGANOX 1035, IRGANOX 1076, IRGANOX 1135, IRGANOX 245, IRGANOX 259, and IRGANOX 295 (all of which are manufactured by BASF), ADK STAB AO-30, and ADK STAB AO. -40, ADK STAB AO-50, ADK STAB AO-60, ADK STAB AO-70, ADK STAB AO-80, ADK STAB AO-90, and ADK STAB AO-330 (all of which are manufactured by ADEKA), Sumilizer GA-80, and Sumizer MDP -S, Sumilizer BBM-S, Sumilizer GM, Sumilizer GS (F), and Sumilizer G (All are manufactured by Sumitomo Chemical Co., Ltd.), HOSTANOX O10, HOSTANOX O16, HOSTANOX O14, and HOSTANOX O3 (all are manufactured by Clariant), Antage BHT, Antage W-300, Antage W-400, and Antage W500 (All as described above, manufactured by Kawaguchi Chemical Industry Co., Ltd.), SEENOX 224M, and SEENOX 326M (all as described above, manufactured by Sipro Kasei Co., Ltd.).

  Examples of the phosphorus antioxidant include cyclohexylphosphine and triphenylphosphine. Commercially available products of the above phosphorus antioxidants include Adeastab PEP-4C, Adeastab PEP-8, Adeastab PEP-24G, Adeastab PEP-36, Adeastab HP-10, Adeastab 2112, Adeastab 260, Adeastab 522A, Adeastab 1178, Adeastab 1500, Adeastab C, Adeastab 135A, Adeastab 3010, and Adeastab TPP (all of which are manufactured by ADEKA), Sandstub P-EPQ, and Hostanox PAR24 (all of which are manufactured by Clariant), and JP-312L, JP -318-0, JPM-308, JPM-313, JPP-613M, JPP-31, JPP-2000PT, and JPH-3800 (all of which are Johoku Manabu Kogyo Co., Ltd.), and the like.

  Examples of the amine-based antioxidant include triethylamine, melamine, ethyldiamino-S-triazine, 2,4-diamino-S-triazine, 2,4-diamino-6-tolyl-S-triazine, and 2,4-diamino- Examples include 6-xylyl-S-triazine and quaternary ammonium salt derivatives.

  The content of the antioxidant (D) is preferably 0.1 parts by weight or more, more preferably 5 parts by weight or more, preferably 50 parts by weight or less with respect to 100 parts by weight of the thermosetting compound (A1). More preferably, it is 30 parts by weight or less. When the content of the antioxidant (D) is not less than the above lower limit and not more than the upper limit, discoloration of the sealing agent is further suppressed in the optical semiconductor device, and a decrease in luminous intensity emitted from the optical semiconductor device is further suppressed. . Furthermore, when the content of the antioxidant (D) is not less than the above lower limit and not more than the upper limit, a molded body that is more excellent in heat resistance can be obtained.

[Other ingredients]
The mold releasability-imparting composition includes a coupling agent, a mold release agent other than the component (C), a resin modifier, a colorant, a diluent, a surface treatment agent, a flame retardant, and a viscosity adjustment, as necessary. An agent, a dispersant, a dispersion aid, a surface modifier, a plasticizer, an antibacterial agent, an antifungal agent, a leveling agent, a stabilizer, an anti-sagging agent or a phosphor may be included. The diluent may be a reactive diluent or a non-reactive diluent.

  It does not specifically limit as said coupling agent, A silane coupling agent and a titanate coupling agent are mentioned.

  The colorant is not particularly limited, and various organic materials such as phthalocyanine, azo compound, disazo compound, quinacridone, anthraquinone, flavantron, perinone, perylene, dioxazine, condensed azo compound, azomethine compound, infrared absorber and ultraviolet absorber. And inorganic pigments such as lead sulfate, chromium yellow, zinc yellow, chromium vermillion, valve shell, cobalt purple, bitumen, ultramarine, carbon black, chromium green, chromium oxide and cobalt green.

(Other details of the mold releasability imparting composition, other details of the molding material, molded product, and method for producing the molded product)
The mold releasability imparting composition comprises a conventionally known method comprising a thermosetting component (A), an inorganic filler (B), a release agent (C), and other components blended as necessary. Obtained by mixing with. The said molding material is obtained by mixing the component mix | blended as needed by a conventionally well-known method.

  A general method for producing the mold releasability imparting composition and the molding material is a method of kneading each component with an extruder, kneader, roll, extruder, etc., and then cooling and pulverizing the kneaded product. Is mentioned. From the viewpoint of improving dispersibility, the kneading of each component is preferably performed in a molten state. The kneading conditions are appropriately determined depending on the type and amount of each component. Kneading is preferably performed at 15 to 150 ° C. for 5 to 120 minutes, more preferably 15 to 150 ° C. for 5 to 100 minutes, further preferably 20 to 100 ° C. for 5 to 60 minutes.

  The mold releasability imparting composition according to the present invention is used to impart releasability to the surface of a mold before molding a molding material to obtain a molded product. The mold releasability imparting composition according to the present invention is preferably molded (dummy molding) before molding the molding material. Using a mold, the mold releasability imparting composition is dummy-molded, and then the mold releasability imparting component derived from the mold releasability imparting composition is removed by removing the dummy molded body. The mold release property of the molded article that is attached to the surface of the molded article and in which the molding material is molded in a later process becomes high.

  The mold releasability imparting composition according to the present invention is used in an optical semiconductor device to obtain a molded body having a frame portion disposed on the side of the optical semiconductor element. The frame is disposed on the side of the optical semiconductor element. It is preferable that the optical semiconductor element and the frame part are separated from each other. The frame part is preferably a frame part filled with a sealant on the inside. The frame portion is preferably a frame portion surrounding a sealant that seals the optical semiconductor element. The frame portion is preferably annular.

  The mold releasability imparting composition according to the present invention is suitably used when a white molding material is obtained by molding a white molding material. By using a white inorganic filler, a white molding material is obtained.

  The mold releasability imparting composition and the molding material are each preferably a tablet.

  In the manufacturing method of the molded object which concerns on this invention, after giving mold release property to the surface of a metal mold | die using the mold release property provision composition mentioned above, a molding material is shape | molded and a molded object is obtained.

  In the method for producing a molded article according to the present invention, after the mold releasability imparting composition is filled in a mold and molded, the molded article molded with the mold releasability imparting composition is taken out. Thus, it is preferable to impart releasability to the surface of the mold.

  In the method for producing a molded body according to the present invention, in the optical semiconductor device, it is preferable to obtain a molded body having a frame portion disposed on the side of the optical semiconductor element. In the manufacturing method of the molded object which concerns on this invention, it is preferable to shape | mold a white molding material and to obtain a white molded object.

  In the optical semiconductor device, the frame portion in the molded body in which the molding material is molded is preferably disposed on a lead frame on which the optical semiconductor element is mounted. The lead frame is, for example, a component for supporting and fixing the optical semiconductor element and achieving electrical connection between the electrode of the optical semiconductor element and external wiring. The molded body is a molded body for an optical semiconductor device, and is preferably an optical semiconductor element mounting substrate.

  In the semiconductor device, the frame portion in the molded body in which the molding material is molded is disposed on the lead frame on which the optical semiconductor element is mounted and on the side of the optical semiconductor element, and light emitted from the optical semiconductor element. It is preferable that the light reflecting portion reflects the light.

  In the semiconductor device, the frame portion in the molded body in which the molding material is molded is disposed on the lead frame on which the optical semiconductor element is mounted so as to surround the optical semiconductor element, and the light emitted from the optical semiconductor element It is preferable to have an inner surface that reflects light. The frame part in the molded body is preferably a frame part surrounding the optical semiconductor element. The molded body is preferably different from a die bond material for bonding (die bonding) an optical semiconductor element in an optical semiconductor device. It is preferable that the molded body does not include the die bond material.

  Examples of the method for obtaining a molded product by molding the mold releasability imparting composition and the molding material include compression molding, transfer molding, lamination molding, injection molding, extrusion molding, and blow molding. It is done. The method for obtaining the molded product by molding the mold releasability imparting composition and the molding material is a compression molding method, a transfer molding method, a layer molding method, an injection molding method, an extrusion molding method or a blow molding method. Is preferred. Of these, transfer molding is preferred. The mold releasability imparting composition according to the present invention is preferably transferred. The mold releasability imparting composition according to the present invention is suitably used before forming a molding material by molding a molding material by transfer molding. In the method for producing a molded body according to the present invention, it is preferable to obtain the molded body by molding the molding material by transfer molding.

  In the transfer molding method, for example, by molding the mold releasability imparting composition and the molding material under the conditions of a molding temperature of 100 to 200 ° C., a molding pressure of 5 to 20 MPa, and a molding time of 60 to 300 seconds, A molded body is obtained.

  It is preferable to obtain a molded body having a lead frame by filling a molding material and putting a lead frame into the mold provided with releasability, and molding the molding material. Such a molded body can be suitably used for an optical semiconductor device.

  Specifically, the molded body can be obtained as follows.

  1 (a) to 1 (e) show molding using a mold releasability imparting composition according to an embodiment of the present invention, imparting releasability to a mold surface, and molding a molding material. It is typical sectional drawing for demonstrating an example of each process of obtaining a body.

  First, the lead frame 22 is placed in the mold 21. Moreover, the mold releasability imparting composition 23 is filled in the mold 21 (FIG. 1A). The mold releasability imparting composition 23 includes a thermosetting component (A), an inorganic filler (B), and a release agent (C). Here, a tablet is used as the mold releasability imparting composition 23.

  Next, the mold releasability imparting composition 23 is molded (FIG. 1B). After the molding, the molded body in which the mold releasability imparting composition 23 is molded is taken out (FIG. 1 (c)). After taking out the molded body in which the mold releasability imparting composition 23 is formed, the releasability imparting component 23 </ b> A contained in the mold releasability imparting composition 23 remains on the surface of the mold 21. . For this reason, releasability is imparted to the surface of the mold 21. In FIGS. 1C to 1E, the thickness of the remaining releasability-imparting component 23A is shown to be thicker than the actual thickness for convenience of illustration.

  Next, the mold 21 is filled with the molding material 24 and the lead frame 22 is inserted (FIG. 1D). Here, a tablet is used as the molding material 24. Next, the molding material 24 is molded (FIG. 1 (e)).

  Thereafter, the molded body in which the molding material 24 is molded is taken out from the mold 21 together with the lead frame 22. Further, the lead frame 22 and the like are cut into a predetermined shape as necessary. The molded body in which the molding material 24 is molded has a frame portion that is disposed on the side of the optical semiconductor element in the optical semiconductor device. The molded body in which the molding material 24 is molded has a bottom. Moreover, an optical semiconductor device can be obtained by filling the inside of the molded body in which the molding material 24 is molded with a sealant. The sealing agent is filled inside the frame portion of the molded body in which the molding material 24 is molded.

(Details of optical semiconductor device and embodiment of optical semiconductor device)
The mold releasability imparting composition according to the present invention is suitably used for obtaining an optical semiconductor device. The optical semiconductor device preferably includes a molded body having a frame portion disposed on the side of the optical semiconductor element. An optical semiconductor device includes a lead frame, an optical semiconductor element mounted on the lead frame, and a molded body having a frame portion disposed on the lead frame, and the molded body is molded from the molding material. It is preferable that the molded body is made.

  In the said optical semiconductor device, it is preferable that the frame part in the said molded object is arrange | positioned at the side of the said optical semiconductor element. Further, in the optical semiconductor device, the frame portion of the molded body is disposed on the side of the optical semiconductor element, and the inner surface of the molded body reflects the light emitted from the optical semiconductor element. It is preferable that

  When a molded body is obtained using the mold releasability imparting composition according to the present invention, a molded body having a frame portion and a bottom portion and having a recess formed between the frame portion and the bottom portion is obtained. It is preferable. It is preferable that the bottom portion is disposed below the frame portion. The frame portion is preferably a frame portion surrounding a sealant that seals the optical semiconductor element. The frame portion is preferably annular.

  It is preferable that the inner surface of the frame portion is inclined toward the side from the lower end to the upper end. It is preferable that the inner surface of the frame portion is inclined toward the side from the bottom side to the side opposite to the bottom portion. The bottom side is the lower end side. The side opposite to the bottom is the upper end side. In the molded body, it is preferable that the opening area of the inner surface of the frame portion increases toward the opening end (upper end).

  By using the mold releasability imparting composition according to the present invention, the molding material can be continuously molded to obtain a molded body. That is, after molding the molding material, the molding material can be molded repeatedly without re-releasing the mold surface. The number of continuous moldings is preferably 100 times or more, more preferably 150 times or more, still more preferably 200 times or more, still more preferably 225 times or more, still more preferably 250 times or more, particularly preferably 275 times or more, and most preferably Is 300 times or more. In the method for producing a molded body according to the present invention, it is preferable to continuously mold 100 times or more. The number of times of continuous molding is more preferably 150 times or more, still more preferably 200 times or more, still more preferably 225 times or more, still more preferably 250 times or more, particularly preferably 275 times or more, and most preferably 300 times or more. It is. The greater the number of times of continuous molding, the higher the manufacturing efficiency of the molded body.

  2A and 2B schematically show an example of an optical semiconductor device including a molded body obtained by molding a molding material using the mold releasability imparting composition according to one embodiment of the present invention. Specifically, a cross-sectional view and a perspective view are shown.

  The optical semiconductor device 1 includes a lead frame 2, an optical semiconductor element 3, and a molded body 4. The optical semiconductor element 3 is preferably a light emitting diode (LED). The molded body 4 has a frame portion 4a and a bottom portion 4b below the frame portion 4a. The frame part 4a is an outer wall part. The frame part 4a is annular.

  In addition, when manufacturing a molded object using the mold release property provision composition which concerns on this invention, you may obtain the molded object which does not have a bottom part. A molded body having a frame part may be molded, and the molded body having the frame part may be used in combination with another bottom member. The molded body having the frame portion may be a frame-shaped molded body having only the frame portion. The bottom member may be a molded body.

  An optical semiconductor element 3 is mounted and arranged on the lead frame 2. A frame portion 4 a is disposed on the lead frame 2. Further, a bottom portion 4 b is disposed between the plurality of lead frames 2 and below the lead frames 2. The optical semiconductor element 3 is disposed inside the frame portion 4a. A frame portion 4 a is disposed on the side of the optical semiconductor element 3. A frame portion 4 a is arranged so as to surround the optical semiconductor element 3. The molded body 4 having the frame portion 4a and the bottom portion 4b is obtained by molding the molding material after imparting mold release properties to the mold surface using the mold mold release property-imparting composition. ing. The molded body 4 is a cured product and is obtained by curing a molding material.

  The inner surface of the frame part 4a has light reflectivity. The frame part 4a is a frame-shaped light reflecting part. Therefore, the periphery of the optical semiconductor element 3 is surrounded by the inner surface of the frame portion 4 a having the light reflectivity of the molded body 4.

  With the end portions on both sides of the frame portion 4a being arranged in the vertical direction, the inner surface of the frame portion 4a is inclined from the lower end (one end) to the upper end (the other end) toward the side. Accordingly, of the light emitted from the optical semiconductor element 3, the light indicated by the arrow B reaching the inner surface of the frame portion 4 a is reflected by the inner surface and travels forward of the optical semiconductor element 3. In the molded body, the upper end of the frame portion 4a is open.

  The optical semiconductor element 3 is connected to the lead frame 2 using a die bond material 5. The die bond material 5 has conductivity. A bonding pad (not shown) provided on the optical semiconductor element 3 and the lead frame 2 are electrically connected by a bonding wire 6. A sealing agent 7 is filled in a region surrounded by the inner surface of the frame portion 4 a of the molded body 4 so as to seal the optical semiconductor element 3 and the bonding wire 6. The frame part 4a and the sealing agent 7 are in contact.

  In the optical semiconductor device 1, when the optical semiconductor element 3 is driven, light is emitted as indicated by a broken line A. In the optical semiconductor device 1, not only the light irradiated from the optical semiconductor element 3 to the side opposite to the upper surface of the lead frame 2, that is, the upper side, but also the light reaching the inner surface of the frame portion 4 a is reflected as indicated by an arrow B. There is also light. Therefore, the brightness of the light extracted from the optical semiconductor device 1 is bright.

  FIG. 3 shows a modification of the optical semiconductor device 1 shown in FIG. The optical semiconductor device 1 shown in FIG. 2 and the optical semiconductor device 11 shown in FIG. 3 differ only in the electrical connection structure using the die bonding materials 5 and 12 and the bonding wires 6 and 13. The die bond material 5 in the optical semiconductor device 1 has conductivity. On the other hand, the optical semiconductor device 11 has a die bond material 12, and the die bond material 12 does not have conductivity. In the optical semiconductor device 1, a bonding pad (not shown) provided on the optical semiconductor element 3 and a lead frame 2 (a lead frame located on the right side in FIG. 2A) are electrically connected by a bonding wire 6. Has been. The optical semiconductor device 11 includes a bonding wire 13 in addition to the bonding wire 6. In the optical semiconductor device 11, a bonding pad (not shown) provided in the optical semiconductor element 3 and a lead frame 2 (lead frame located on the right side in FIG. 3) are electrically connected by a bonding wire 6. Further, a bonding pad (not shown) provided on the optical semiconductor element 3 and the lead frame 2 (lead frame located on the left side in FIG. 3) are electrically connected by a bonding wire 13.

  The structures shown in FIGS. 2 and 3 are merely examples of the optical semiconductor device, and the structure of the molded body and the mounting structure of the optical semiconductor element can be appropriately modified.

  Hereinafter, the present invention will be clarified by giving specific examples and comparative examples of the present invention. The present invention is not limited to the following examples.

  In the examples and comparative examples, the following materials were used.

(Thermosetting compound (A1))
1) YD-011 (bisphenol A type epoxy resin, epoxy equivalent 470, manufactured by Nippon Steel Chemical Co., Ltd.)
2) YD-012 (bisphenol A type epoxy resin, epoxy equivalent 650, manufactured by Nippon Steel Chemical Co., Ltd.)
3) YDCN-704 (cresol novolac type epoxy resin, epoxy equivalent 210, manufactured by Nippon Steel Chemical Co., Ltd.)
4) YDPN-638 (phenol novolac type epoxy resin, epoxy equivalent 180, manufactured by Nippon Steel Chemical Co., Ltd.)

(Curing agent (A2))
1) HF-1M (phenol novolac curing agent, curing agent equivalent 105, manufactured by Meiwa Kasei Co., Ltd.)
2) HF-4M (phenol novolac curing agent, curing agent equivalent 105, manufactured by Meiwa Kasei Co., Ltd.)

(Curing accelerator (A3))
1) TPP (triphenylphosphine, manufactured by Wako Pure Chemical Industries, Ltd.)

(Spherical filler (B1))
1) MSR-3500 (spherical silica, average particle size 30 μm, manufactured by Tatsumori)

(Fracture filler (B2))
1) 3K-S (crushed silica, average particle size 35 μm, manufactured by Tatsumori)
2) NX-7 (crushed silica, average particle size 13 μm, manufactured by Tatsumori)

(Fatty acid ester wax (C1))
1) Lycowax E (Montanic acid ester, manufactured by Clariant)
2) M-9676 (stearic acid ester, manufactured by NOF Corporation)

(Oxidized or non-oxidized polyolefin wax (C2))
1) Rico wax PED191 (polyethylene oxide wax, manufactured by Clariant)
2) Rico wax PE520 (polyethylene wax, manufactured by Clariant)
3) NP055 (polypropylene wax, manufactured by Mitsui Chemicals)

(Other mold release agents)
1) Diamond 200 (Monoamide, manufactured by Nippon Kasei Co., Ltd.)
2) SLIPAX ZHS (Bisamide, Nippon Kasei Co., Ltd.)
3) GF-200 (metal soap, NOF Corporation)

(Antioxidant (D))
1) Irganox 1035 (phenolic antioxidant, manufactured by BASF)

(Examples 1-22 and Comparative Examples 1-9)
Each component shown in the following Tables 1 to 3 is blended in the blending amounts shown in the following Tables 1 to 3 (the blending unit is parts by weight), and is 80 ° C. with a mixer (Laboplast Mill R-60, manufactured by Toyo Seiki Seisakusho). And kneaded for 10 minutes to obtain a kneaded product. The obtained kneaded product was pulverized and then tableted to obtain a mold releasability imparting composition.

(Evaluation)
(1) Number of continuous moldings (release properties)
Molding material preparation:
30 parts by weight of Celoxide 2021P (3,4-epoxycyclohexenylmethyl-3 ′, 4′-epoxycyclohexene carboxylate, epoxy equivalent 126, manufactured by Daicel) and EHPE3150 (epoxy resin having an alicyclic skeleton, epoxy equivalent 177) 70 parts by weight of Daicel), 82 parts by weight of Ricacid MH-700 (a mixture of hexahydrophthalic anhydride and methylhexahydrophthalic anhydride, manufactured by Shin Nippon Rika), CR-90 (rutile titanium oxide, 300 parts by weight of surface treated with Al and Si, manufactured by Ishihara Sangyo Co., Ltd., MSR-3512 (spherical silica, average particle size 30 μm, manufactured by Tatsumori Co., Ltd.) 600 parts by weight, CMC-12 (crushed silica, average Blended with 100 parts by weight of 5 μm particle size, 2-5 aspect ratio, manufactured by Tatsumori Co., Ltd. Mill R-60, were mixed Toyo Seiki Seisakusho) for 15 minutes to obtain a molding material.

Continuous molding:
A circuit was formed on a copper material (TAMAC 194) by etching and then silver plating was performed to obtain a lead frame having a thickness of 0.2 mm. As a transfer molding apparatus, “YPS-MP” manufactured by TOWA was used. As a mold, a collective molding die having 150 concave portions (optical semiconductor element mounting portions) arranged in a matrix of 15 vertical × 10 horizontal was used.

  First, using a melamine resin cleaning material (“EMEC3” manufactured by Sumitomo Bakelite Co., Ltd.) for cleaning the mold surface, molding was performed three times to clean the mold surface.

  Next, molding was performed three times using the obtained mold releasability imparting composition, a mold release treatment was performed, and mold releasability was imparted to the mold.

  Subsequently, using the obtained molding material under conditions of a molding temperature of 170 ° C., an injection pressure of 7 MPa, and a molding time of 3 minutes, a mounting substrate for an optical semiconductor device is repeatedly molded on the lead frame by transfer molding. The number of shots (the number of continuous moldings) until was attached to the mold was examined.

(2) Reflow resistance The mounting substrate for optical semiconductor devices obtained by the evaluation of the above (1) continuous molding was prepared. This mounting substrate for an optical semiconductor device was after-cured at 170 ° C. for 2 hours. In the molded article after the after-curing, when there was a burr, the burr was removed using AX-930 (manufactured by Rix Corporation).

  Next, a blue light-emitting element of a sapphire substrate having InGaN as a light-emitting layer was placed on the molded body after the after-curing using a silicone resin adhesive. The light emitting element and the lead frame were electrically connected using a gold wire having a diameter of 30 μm. A sealing agent was dropped into each of the concave portions of the molded body on which the light emitting element was placed on the bottom surface. The sealant contains 100 parts by weight of silicone resin and 30 parts by weight of YAG phosphor. After the dropping, the sealant was cured at 150 ° C. for 3 hours. Finally, it was cut out from the lead frame to obtain an optical semiconductor device emitting white light.

  The obtained white light emitting optical semiconductor device was allowed to stand for 24 hours under conditions of a temperature of 85 ° C. and a humidity of 85%, and then a reflow test was performed in an air atmosphere. “SNR-825GT” manufactured by SMIC was used as the reflow furnace. The upper limit temperature of reflow was set to 260 ° C. The presence or absence of peeling of the sealant from the molded product was observed, and the reflow resistance was determined according to the following criteria.

[Judgment criteria for reflow resistance]
XX: No peeling is observed even if the reflow test is repeated three times. XX: No peeling is observed in the second reflow test, but peeling is observed in the third reflow test. No peeling is seen in the reflow test, but peeling is seen in the second reflow test. X: peeling is seen in the first reflow test.

(3) Luminance retention A white light-emitting optical semiconductor device (before reflow test) obtained by (2) evaluation of reflow resistance was prepared. The light intensity (light intensity before energization test) of this optical semiconductor device was measured using OL770 (manufactured by Optronic Laboratories). Then, after energizing for 500 hours at a current of 120 mA under the conditions of a temperature of 85 ° C. and a humidity of 85%, the light intensity of the optical semiconductor device (light intensity after energization test) was measured. The luminous intensity retention was determined from the luminous intensity before and after the energization test. The luminous intensity retention was determined according to the following criteria.

  The luminous intensity retention is represented by the following formula.

Luminance retention rate (%) = (Luminance after energization test) / (Luminance before energization test) × 100
[Criteria for luminous intensity retention]
○: Luminance retention rate is 90% or more ×: Luminance retention rate is less than 90%

  The results are shown in Tables 1 to 3 below. In the following Tables 1 to 3, the contents of (C1) and (C2) indicate the contents in 100% by weight of the mold releasability imparting composition. In Comparative Example 1, since molding was impossible, (2) reflow resistance and (3) light intensity retention were not evaluated.

DESCRIPTION OF SYMBOLS 1 ... Optical semiconductor device 2 ... Lead frame 3 ... Optical semiconductor element 4 ... Molding body 4a ... Frame part 4b ... Bottom part 5 ... Die bond material 6 ... Bonding wire 7 ... Sealant 11 ... Optical semiconductor device 12 ... Die bond material 13 ... Bonding Wire 21 ... Mold 22 ... Lead frame 23 ... Mold mold release imparting composition 23A ... Mold release imparting component 24 ... Molding material

Claims (14)

A mold releasability imparting composition used to impart releasability to the surface of a mold before molding a molding material to obtain a molded body,
Including a thermosetting component, an inorganic filler, and a release agent;
A mold releasability imparting composition, wherein the release agent contains both a fatty acid ester wax and an oxidized or non-oxidized polyolefin wax.   In 100% by weight of the mold releasability imparting composition, the content of the fatty acid ester wax is 0.5% by weight or more and 3% by weight or less, and the content of the oxidized or non-oxidized polyolefin wax is 1. The mold releasability imparting composition according to claim 1, wherein the composition is at least 9% by weight and not more than 9% by weight.   The mold releasability imparting composition according to claim 1 or 2, wherein the inorganic filler is silica.   The mold releasability imparting composition according to any one of claims 1 to 3, wherein the inorganic filler contains both a spherical filler and a crushed filler.   The mold releasability imparting composition according to any one of claims 1 to 4, wherein the thermosetting component contains an epoxy compound and a curing agent.   The mold releasability imparting composition according to any one of claims 1 to 5, wherein the thermosetting component contains a curing accelerator.   The mold releasability imparting composition according to any one of claims 1 to 6, wherein the thermosetting component contains both a bisphenol A type epoxy compound and a novolac type epoxy compound.   The mold releasability imparting composition according to any one of claims 1 to 7, which is used before forming a molding material by transfer molding to obtain a molded body.   The mold releasability imparting composition according to any one of claims 1 to 8, which is used in an optical semiconductor device to obtain a molded body having a frame portion disposed on a side of an optical semiconductor element.   The mold releasability imparting composition according to any one of claims 1 to 9, which is used before a white molding material is molded to obtain a white molded body.   Molding, wherein a mold release property is imparted to the surface of the mold using the mold release property imparting composition according to any one of claims 1 to 10, and then a molding material is molded to obtain a molded body. Body manufacturing method.   The manufacturing method of the molded object of Claim 11 which shape | molds the said molding material by transfer molding and obtains a molded object.   The manufacturing method of the molded object of Claim 11 or 12 which obtains the molded object which has a frame part arrange | positioned in the optical semiconductor device at the side of an optical semiconductor element.   The manufacturing method of the molded object of any one of Claims 11-13 which shape | molds a white molding material and obtains a white molded object.

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