TWI845486B - Epoxy resin composition for sealing and electronic component apparatus - Google Patents

Abstract

A epoxy resin composition for sealing includes (A) an epoxy resin, (B) a curing agent, (C) a curing accelerator, (D) inorganic fillers, and (E) a fatty acid amide compound having a carbon number of from 17 to 50, and a content of the (D) inorganic fillers is more than 80 % by volume with respect to the total amount of the composition.

Description

Sealing epoxy resin composition and electronic component device

The present invention relates to a sealing epoxy resin composition and an electronic component device.

In recent years, in the pursuit of higher-level, thinner, and smaller electronic devices, semiconductor components have been increasingly integrated and functionalized. As a result, the requirements for epoxy resin compositions for sealing have become increasingly stringent. In particular, as semiconductor devices are becoming thinner and multi-pin, the flow path of the epoxy resin composition in the molding die becomes extremely narrow when the semiconductor components are sealed, so an epoxy resin composition with better fluidity is required. In addition, due to the higher functionality of semiconductor components, the heat generated by the components themselves increases, and there are concerns about malfunctions and reduced component life. Therefore, it is ideal to have excellent thermal conductivity after the epoxy resin composition is cured.

As a method for improving the thermal conductivity of an epoxy resin composition after curing, a method of increasing the amount of a thermally conductive filler in the epoxy resin composition has been reported (for example, refer to Patent Document 1). [Prior Art Document] [Patent Document]

[Patent Document 1] Japanese Patent Publication No. 2012-211225

[Problem to be solved by the invention] However, when an inorganic filler such as a thermal conductive filler is blended into an epoxy resin composition, the fluidity of the epoxy resin composition decreases. Furthermore, when a large amount of the inorganic filler is blended into the epoxy resin composition, the decrease in the fluidity of the epoxy resin composition becomes more significant. Therefore, it is desirable to suppress the decrease in fluidity when an inorganic filler is blended into an epoxy resin composition.

One aspect of the present invention aims to provide a sealing epoxy resin composition having excellent fluidity, and an electronic component device including a component sealed using the epoxy resin composition. [Means for solving the problem]

Means for solving the above-mentioned problems include the following implementation methods. ＜1＞ A sealing epoxy resin composition comprising (A) an epoxy resin, (B) a hardener, (C) a hardening accelerator, (D) an inorganic filler, and (E) a fatty acid amide compound having 17 to 50 carbon atoms, wherein the content of the (D) inorganic filler exceeds 80% by volume relative to the total amount of the composition. ＜2＞ The sealing epoxy resin composition as described in ＜1＞, wherein the (D) inorganic filler comprises aluminum oxide. ＜3＞ The sealing epoxy resin composition as described in ＜2＞, wherein the content of the aluminum oxide exceeds 80% by volume relative to the total amount of the composition. <4> The sealing epoxy resin composition as described in any one of <1> to <3>, wherein the content of the fatty acid amide compound (E) having 17 to 50 carbon atoms is 0.005% by mass to 1.0% by mass relative to the total amount of the composition. <5> The sealing epoxy resin composition according to any one of <1> to <4>, wherein the (E) fatty acid amide compound having 17 to 50 carbon atoms comprises at least one compound selected from the group consisting of oleamide, stearamide, erucamide, ethylenebisoleamide, hexamethylenebisoleamide, dioleyl adipamide, methylenebiserucamide, ethylenebiserucamide, hexamethylenebiserucamide, meta-xylenebiserucamide, para-phenylenebiserucamide, methylenebistearate, and ethylenebislaurate.

<6> An electronic component device comprising a component and a cured product of the sealing epoxy resin composition described in any one of <1> to <5> for sealing the component. [Effect of the invention]

According to the present disclosure, a sealing epoxy resin composition having excellent fluidity and an electronic component device including a component sealed using the same can be provided.

The following is a detailed description of the embodiments for implementing the present invention. However, the present invention is not limited to the following embodiments. In the following embodiments, the constituent elements (including element steps, etc.) are not required unless otherwise specified. The same is true for numerical values and their ranges, which do not limit the present invention.

In this disclosure, the numerical range represented by "～" includes the numerical values recorded before and after "～" as the minimum and maximum values, respectively. In the numerical range recorded in stages in this disclosure, the upper limit or lower limit recorded in one numerical range can also be replaced by the upper limit or lower limit of another numerical range recorded in stages. In addition, in the numerical range recorded in this disclosure, the upper limit or lower limit of the numerical range can also be replaced by the value shown in the embodiment. In this disclosure, each component can also contain multiple equivalent substances. When there are multiple substances equivalent to each component in the composition, the content rate of each component refers to the total content rate of the multiple substances present in the composition unless otherwise specified.

[Sealing epoxy resin composition] The sealing epoxy resin composition disclosed herein comprises (A) epoxy resin, (B) curing agent, (C) curing accelerator, (D) inorganic filler and (E) fatty acid amide compound having 17 to 50 carbon atoms, wherein the content of the inorganic filler (D) exceeds 80% by volume relative to the total amount of the composition. Thus, a sealing epoxy resin composition having excellent fluidity can be provided, and since the content of the inorganic filler (D) exceeds 80% by volume, there is a tendency that the thermal conductivity of the cured product is excellent. In addition, the sealing epoxy resin composition disclosed herein is used, for example, for sealing electronic component devices.

[(A) Epoxy resin] The epoxy resin composition for sealing disclosed herein (hereinafter, also referred to as "epoxy resin composition") includes (A) epoxy resin. The type of (A) epoxy resin is not particularly limited as long as it has an epoxy group in the molecule.

Specifically, the epoxy resin (A) may be a phenolic varnish obtained by condensing or co-condensing at least one phenolic compound selected from the group consisting of phenolic compounds such as phenol, cresol, xylenol, resorcinol, o-catechol, bisphenol A, bisphenol F, and naphthol compounds such as α-naphthol, β-naphthol, and dihydroxynaphthalene with an aliphatic aldehyde compound such as formaldehyde, acetaldehyde, and propionaldehyde under an acidic catalyst. a phenolic varnish type epoxy resin (phenol phenolic varnish type epoxy resin, o-cresol phenolic varnish type epoxy resin, etc.) obtained by epoxidizing the phenolic varnish resin; a triphenylmethane type phenolic resin obtained by condensing or co-condensing the above-mentioned phenolic compound with an aromatic aldehyde compound such as benzaldehyde or salicylic aldehyde under an acidic catalyst and epoxidizing the triphenylmethane type phenolic resin; Alkyl-type epoxy resins; copolymerized epoxy resins obtained by epoxidizing a novolac resin obtained by co-condensing the above-mentioned phenolic compounds and naphthol compounds with an aldehyde compound such as formaldehyde, acetaldehyde, propionaldehyde, benzaldehyde, and salicylic aldehyde under an acidic catalyst; diphenylmethane-type epoxy resins as diglycidyl ethers of bisphenol A, bisphenol AD, bisphenol F, etc.; alkyl-substituted or non-alkyl-substituted Biphenyl type epoxy resins of diglycidyl ethers of substituted biphenols; stilbene type epoxy resins of diglycidyl ethers of stilbene phenol compounds; sulfur-containing epoxy resins of diglycidyl ethers of bisphenol S, etc.; epoxy resins of glycidyl ethers of alcohols such as butanediol, polyethylene glycol, and polypropylene glycol; polyols such as phthalic acid, isophthalic acid, tetrahydrophthalic acid, dimer acid, etc. Glycidyl ester epoxy resin of glycidyl ester of carboxylic acid compound; glycidylamine epoxy resin obtained by replacing the active hydrogen bonded to the nitrogen atom of aniline, diaminodiphenylmethane, isocyanuric acid, etc. with glycidyl group; dicyclopentadiene epoxy resin obtained by epoxidizing the co-condensation resin of dicyclopentadiene and phenol compound; dicyclopentadiene epoxy resin obtained by epoxidizing the olefinic bond in the molecule; Alicyclic epoxy resins such as epoxide vinyl cyclohexene, 3,4-epoxycyclohexylmethyl-3,4-epoxycyclohexane carboxylate, 2-(3,4-epoxy)cyclohexyl-5,5-spiro(3,4-epoxy)cyclohexane-m-dioxane; p-xylene-modified epoxy resin as glycidyl ether of p-xylene-modified phenol resin; glycidyl ether of m-xylene-modified phenol resin meta-xylene modified epoxy resin; terpene modified epoxy resin as the glycidyl ether of terpene modified phenol resin; dicyclopentadiene modified epoxy resin as the glycidyl ether of dicyclopentadiene modified phenol resin; cyclopentadiene modified epoxy resin as the glycidyl ether of cyclopentadiene modified phenol resin; polycyclic aromatic ring modified epoxy resin as the glycidyl ether of polycyclic aromatic ring modified phenol resin; Naphthalene-type epoxy resins which are glycidyl ethers of phenol resins containing naphthalene rings; halogenated phenol novolac-type epoxy resins; hydroquinone-type epoxy resins; trihydroxymethylpropane-type epoxy resins; linear aliphatic epoxy resins obtained by oxidizing olefinic bonds with peracids such as peracetic acid; aralkyl-type epoxy resins obtained by epoxidizing aralkyl-type phenol resins such as phenol aralkyl resins and naphthol aralkyl resins, etc. Furthermore, epoxides of silicone resins, epoxides of acrylic resins, etc. can also be listed as epoxy resins. These epoxy resins can be used alone or in combination of two or more.

(A) The epoxy equivalent (molecular weight/number of epoxy groups) of the epoxy resin is not particularly limited. From the viewpoint of balancing various properties such as formability, reflow resistance, and electrical reliability, it is preferably 100 g/eq to 1000 g/eq, and more preferably 150 g/eq to 500 g/eq.

The epoxy equivalent of the epoxy resin (A) is a value measured by a method in accordance with Japanese Industrial Standards (JIS) K 7236:2009.

When the epoxy resin (A) is solid, its melting point or softening point is not particularly limited. From the viewpoint of moldability and reflow resistance, it is preferably 40°C to 180°C, and from the viewpoint of workability during preparation of the epoxy resin composition, it is more preferably 50°C to 130°C.

The melting point of the epoxy resin (A) is a value measured by differential scanning calorimetry (DSC), and the softening point of the epoxy resin is a value measured by a method (globe method) in accordance with JIS K 7234:1986.

From the viewpoints of strength, fluidity, heat resistance, moldability, etc., the content of the epoxy resin (A) in the epoxy resin composition is preferably 0.5 mass % to 30 mass %, more preferably 2 mass % to 20 mass %, further preferably 3 mass % to 15 mass %, and particularly preferably 5 mass % to 10 mass %.

[(B) Hardener] The epoxy resin composition disclosed herein includes a (B) hardener. The type of hardener is not particularly limited and can be selected based on the type of (A) epoxy resin, the desired properties of the epoxy resin composition, etc.

Specific examples of the (B) hardener include phenol hardeners, amine hardeners, acid anhydride hardeners, polythiol hardeners, polyaminoamide hardeners, isocyanate hardeners, blocked isocyanate hardeners, etc. From the viewpoint of improving heat resistance, the hardener is preferably a phenol hardener.

As the phenol curing agent, specifically, there can be mentioned: a novolac type phenol resin obtained by condensing or co-condensing at least one phenolic compound selected from the group consisting of phenolic compounds such as resorcinol, o-catechol, bisphenol A, bisphenol F, phenol, cresol, xylenol, phenylphenol, aminophenol, and naphthol compounds such as α-naphthol, β-naphthol, and dihydroxynaphthalene with an aldehyde compound such as formaldehyde, acetaldehyde, propionaldehyde, benzaldehyde, and salicylic aldehyde under an acidic catalyst; Aralkyl phenol resins such as phenol aralkyl resins and naphthol aralkyl resins synthesized from methoxy-p-xylene, bis(methoxymethyl)biphenyl, etc.; p-xylene-modified phenol resins; m-xylene-modified phenol resins; melamine-modified phenol resins; terpene-modified phenol resins; dicyclopentadiene-type phenol resins and dicyclopentadiene-type naphthol resins synthesized by copolymerization of the above-mentioned phenolic compounds with dicyclopentadiene; cyclopentadiene-modified phenol resins; polycyclic aromatic ring-modified phenol resins; biphenyl-type phenol resins, etc. These phenol curing agents may be used alone or in combination of two or more.

(B) The functional group equivalent weight of the hardener (hydroxyl group equivalent weight in the case of a phenol hardener) is not particularly limited. From the viewpoint of balancing various properties such as formability, reflow resistance, and electrical reliability, it is preferably 70 g/eq to 1000 g/eq, and more preferably 80 g/eq to 500 g/eq.

The hydroxyl equivalent of the phenol curing agent is set to a value measured by a method in accordance with JIS K 0070:1992.

When the (B) curing agent is solid, its melting point or softening point is not particularly limited. From the viewpoint of formability and reflow resistance, it is preferably 40°C to 180°C, and from the viewpoint of operability during the production of the epoxy resin composition, it is more preferably 50°C to 130°C.

The melting point or softening point of the (B) hardener is set to a value measured in the same manner as the melting point or softening point of the epoxy resin.

The equivalent ratio of the (A) epoxy resin to the (B) hardener, that is, the ratio of the number of functional groups in the (B) hardener to the number of functional groups in the (A) epoxy resin (number of functional groups in the (B) hardener/number of functional groups in the (A) epoxy resin) is not particularly limited. From the viewpoint of reducing the amount of each unreacted component, it is preferably set in the range of 0.5 to 1.5, more preferably in the range of 0.6 to 1.3, and further preferably in the range of 0.7 to 1.2.

[(C) Hardening accelerator] The epoxy resin composition disclosed herein includes a (C) hardening accelerator. The type of the hardening accelerator is not particularly limited and can be selected based on the type of the (A) epoxy resin, the desired properties of the epoxy resin composition, etc.

(C) The hardening accelerator includes, specifically, tertiary amines such as 1,8-diaza-bicyclo (5,4,0) undecene-7, 1,5-diaza-bicyclo (4,3,0) nonene, 5,6-dibutylamino-1,8-diaza-bicyclo (5,4,0) undecene-7, benzyldimethylamine, triethanolamine, dimethylaminoethanol, tris (dimethylaminomethyl) phenol, and their derivatives; imidazoles such as 2-methylimidazole, 2-phenylimidazole, 2-phenyl-4-methylimidazole, and their derivatives. derivatives; organic phosphines such as tributylphosphine, methyldiphenylphosphine, triphenylphosphine, diphenylphosphine, phenylphosphine, and compounds with intramolecular polarization formed by adding compounds having π bonds such as maleic anhydride, benzoquinone, and diazonophenylmethane to these phosphines; tetraphenylphosphonium tetraphenylborate, triphenylphosphine tetraphenylborate, 2-ethyl-4-methylimidazolium tetraphenylborate, N-methyltetraphenylphosphonium tetraphenylborate, adducts of triphenylphosphine and benzoquinone, adducts of tri-p-toluenephosphine and benzoquinone, triphenylphosphonium triphenylborane, and the like. These hardening accelerators may be used alone or in combination of two or more.

The content of the (C) curing accelerator in the epoxy resin composition is not particularly limited as long as the curing acceleration effect can be obtained. The content of the (C) curing accelerator in the epoxy resin composition is, for example, preferably 0.1% by mass to 8.0% by mass, more preferably 0.5% by mass to 5.0% by mass, further preferably 1.0% by mass to 4.0% by mass, and particularly preferably 1.0% by mass to 3.0% by mass, relative to the total amount of the (A) epoxy resin and the (B) curing agent. When the content of the (C) curing accelerator is 0.1 mass % or more relative to the total amount of the (A) epoxy resin and the (B) curing agent, there is a tendency that the curing time can be shortened, and when it is 8.0 mass % or less, there is a tendency that the curing speed is not too fast and a good molded product can be obtained.

[(D) Inorganic filler] The epoxy resin composition disclosed herein includes (D) an inorganic filler. By including (D) an inorganic filler, it is possible to achieve reduced hygroscopicity and improved strength when a cured product is produced. Furthermore, in the epoxy resin composition disclosed herein, the content of (D) an inorganic filler exceeds 80% by volume relative to the total amount of the composition. This can improve the thermal conductivity when the epoxy resin composition is produced into a cured product.

From the viewpoint of thermal conductivity when the cured product is obtained, the content of the (D) inorganic filler in the epoxy resin composition of the present disclosure is preferably 81 volume % or more, more preferably 83 volume % or more, and even more preferably 84 volume % or more, relative to the total amount of the composition.

In addition, from the viewpoint of fluidity, in the epoxy resin composition disclosed herein, the content of the (D) inorganic filler is preferably 90 volume % or less, more preferably 87 volume % or less, and even more preferably 86 volume % or less, relative to the total amount of the composition.

From the viewpoint of improving the thermal conductivity when the epoxy resin composition is cured, the (D) inorganic filler preferably contains aluminum oxide.

From the viewpoint of thermal conductivity when the cured product is obtained, the content of aluminum oxide in the epoxy resin composition disclosed herein is preferably more than 80 volume %, more preferably 81 volume % or more, further preferably 83 volume % or more, and particularly preferably 84 volume % or more relative to the total amount of the composition.

In addition, from the viewpoint of fluidity, in the epoxy resin composition disclosed herein, the content of aluminum oxide relative to the total amount of the composition is preferably 90 volume % or less, more preferably 87 volume % or less, and even more preferably 86 volume % or less.

From the viewpoint of further improving the thermal conductivity when the epoxy resin composition is made into a cured product, the content of alumina in the (D) inorganic filler is preferably 70 volume % or more, more preferably 75 volume % or more, further preferably 85 volume % or more, particularly preferably 90 volume % to 100 volume %, further preferably 95 volume % to 100 volume %. The content of alumina in the (D) inorganic filler may be 97 volume % to 99.9 volume %, or may be 98.5 volume % to 99.5 volume % relative to the total amount of the (D) inorganic filler.

(D) The inorganic filler may include an inorganic filler other than aluminum oxide. As the inorganic filler other than aluminum oxide, it is preferred to include at least one inorganic filler (specific inorganic filler) selected from the group consisting of silicon dioxide, silicon nitride, boron nitride, magnesium oxide, zinc oxide, silicon carbide and aluminum nitride.

(D) Inorganic fillers may include other inorganic fillers other than the aforementioned specific inorganic fillers as inorganic fillers other than alumina. Examples of other inorganic fillers include fused silica, crystalline silica, zircon, calcium silicate, calcium carbonate, potassium titanate, ceria, zirconium oxide, forsterite, steatite, spinel, andalusite, titanium dioxide and other powders or spherical particles thereof, single crystal fibers such as potassium titanate, glass fibers, polyaramide fibers, carbon fibers, and the like. Among them, fused silica is preferred from the viewpoint of reducing the linear expansion coefficient. In addition, from the viewpoint of flame retardant effect, other inorganic fillers include aluminum hydroxide, zinc borate, magnesium hydroxide, etc. Other inorganic fillers may be used alone or in combination of two or more.

The content of the inorganic filler other than alumina in the (D) inorganic filler may be 30 volume % or less, 15 volume % or less, 10 volume % or less, 5 volume % or less, 0.1 volume % to 3 volume % or less, or 0.5 volume % to 1.5 volume % or less, based on the total amount of the (D) inorganic filler.

From the viewpoints of hygroscopicity, reduction in linear expansion coefficient, improvement in strength and solder heat resistance, the content of the (D) inorganic filler in the epoxy resin composition is preferably 75% by mass to 97% by mass, more preferably 80% by mass to 95% by mass, and even more preferably 85% by mass to 92% by mass, based on the total amount of the composition.

The shape of the (D) inorganic filler is not particularly limited, and may be powdery, spherical, fibrous, etc. Among them, a spherical shape is preferred from the viewpoint of fluidity during molding of the epoxy resin composition and mold wear.

[(E) fatty acid amide compound having 17 to 50 carbon atoms] The epoxy resin composition disclosed herein contains (E) fatty acid amide compound having 17 to 50 carbon atoms. By containing (E) fatty acid amide compound having 17 to 50 carbon atoms, the fluidity of the epoxy resin composition is improved. Furthermore, it is speculated that the improvement in the fluidity of the epoxy resin composition is due to the fact that (E) fatty acid amide compound having 17 to 50 carbon atoms improves the dispersibility of (A) epoxy resin, (D) inorganic filler, etc. More specifically, the following speculation is made. First, the fatty acid amide compound (E) having 17 to 50 carbon atoms contains a group having affinity with the resin component and a group having excellent adsorption with the (D) inorganic filler, whereby the group having excellent adsorption with the (D) inorganic filler is adsorbed to the (D) inorganic filler, and the wettability between the resin component and the (D) inorganic filler is improved by the action of the group having affinity with the resin component. It is considered that, even when the content of the (D) inorganic filler is increased to achieve high filling, the aggregation of the (D) inorganic filler is suppressed, the dispersibility of the (D) inorganic filler is improved, and the fluidity of the epoxy resin composition is improved.

(E) The fatty acid amide compound having 17 to 50 carbon atoms may specifically include monoamides such as oleamide, stearamide, and erucamide; and diamides such as ethylenebisoleamide, hexamethylenebisoleamide, dioleyl adipamide, methylenebiserucamide, ethylenebiserucamide, hexamethylenebiserucamide, meta-xylenebiserucamide, p-phenylenebiserucamide, methylenebistearate, and ethylenebislaurate. The fatty acid amide compound having 17 to 50 carbon atoms may be used alone or in combination of two or more. Among them, oleamide, ethylenebisoleamide and methylenebistearate amide are preferred from the viewpoint of fluidity.

By using a fatty acid amide compound having 17 or more carbon atoms, the compatibility with the epoxy resin (A) tends to be suppressed from becoming too high, and the reduction in mold release properties from the mold due to the generation of curing resistance tends to be suppressed. Furthermore, the water absorption rate of the cured product of the epoxy resin composition tends to be increased, and there is a tendency to suppress the adverse effect on solder crack resistance.

By using a fatty acid amide compound having a carbon number of 50 or less, there is a tendency to suppress a decrease in compatibility with the epoxy resin (A) and a decrease in fluidity. Furthermore, there is a tendency to suppress mold contamination and a decrease in adhesion to the substrate caused by the fatty acid amide compound seeping out from the epoxy resin composition during molding.

Furthermore, the carbon number in the fatty acid amide compound refers to the carbon number of the hydrocarbon part in the compound, and is assumed to exclude the carbon number of the amide group. In addition, the hydrogen of the hydrocarbon part may be substituted with another functional group. When the hydrogen of the hydrocarbon part is substituted with another functional group, and the substituent has carbon atoms, the carbon number of the substituent is assumed to be not included in the carbon number of the fatty acid amide compound.

In addition, the (E) fatty acid amide compound having 17 to 50 carbon atoms may be an unsaturated fatty acid amide having a double bond or a saturated fatty acid amide not having a double bond. The (E) fatty acid amide compound having 17 to 50 carbon atoms may have an aromatic ring in the molecule or may not have an aromatic ring.

The content of the fatty acid amide compound having 17 to 50 carbon atoms (E) in the epoxy resin composition is not particularly limited. For example, from the viewpoint of fluidity, it may be 0.005% to 1.0% by mass, 0.01% to 1.0% by mass, 0.02% to 1.0% by mass, 0.1% to 0.8% by mass, or 0.3% to 0.7% by mass, relative to the total amount of the composition. In addition, the content of the fatty acid amide compound having 17 to 50 carbon atoms (E) in the epoxy resin composition may be 0.5% by mass or less, 0.4% by mass or less, or 0.3% by mass or less, relative to the total amount of the composition.

In addition, the epoxy resin composition may contain a fatty acid amide compound having 16 or less carbon atoms, or may contain a fatty acid amide compound having 51 or more carbon atoms, within the range where the effect of the present invention is exerted.

[Other components] The epoxy resin composition disclosed herein may also contain other components besides the aforementioned (A) epoxy resin, (B) hardener, (C) hardening accelerator, (D) inorganic filler and (E) fatty acid amide compound having 17 to 50 carbon atoms. As other components, there is no particular limitation within the scope of exerting the effect of the present invention, and examples thereof include: release agents such as wax, fatty acid esters, and fatty acid metal salts; coupling agents such as silane coupling agents and titanium ester coupling agents; flame retardants such as brominated epoxy resins and phosphorus compounds; flame retardant additives such as antimony trioxide and antimony tetroxide; coloring agents such as carbon black and iron oxide; stress relievers such as silicone oil, silicone rubber, and synthetic rubber; and various additives such as antioxidants.

[Method for preparing epoxy resin composition] The method for preparing epoxy resin composition is not particularly limited. As a general method, the following method can be cited: after the prescribed amount of ingredients is fully mixed by a mixer, etc., melt-kneading is performed by a mixing roll, an extruder, etc., cooling and pulverizing. More specifically, for example, the following method can be cited: the prescribed amount of the above ingredients is stirred and mixed, kneaded by a kneader, a roll, an extruder (extruder), etc. preheated to 70°C to 140°C, cooling and pulverizing.

[Electronic component device] The electronic component device disclosed herein includes a component and a cured product of the above-mentioned sealing epoxy resin composition that seals the component. As the electronic component device, there can be cited a device obtained by sealing the following component parts using an epoxy resin composition, wherein the component parts are obtained by mounting components (active components such as semiconductor chips, transistors, diodes, gates, etc., passive components such as capacitors, resistors, coils, etc.) on supporting members such as lead frames, wired conveying tapes, wiring boards, glass, silicon wafers, and organic substrates. More specifically, they include: Dual Inline Package (DIP), Plastic Leaded Chip Carrier (PLCC), Quad Flat Package (QFP), Small Outline Package (SOP), Small Outline J-lead package (SOJ), Thin Small Outline Package (TSOP), Thin Quad Flat Package (TQFP), and other general resin-sealed integrated circuits (ICs), which have a structure in which the component is fixed on a lead frame and the terminal and lead portions of the component such as bonding pads are connected by wire bonding, bumps, etc., and then sealed using an epoxy resin composition by transfer molding, etc.; Tape Carrier (TCP) Package (TCP), which has a structure in which components connected to a conveying tape by bumps are sealed with an epoxy resin composition; Chip On Board (COB) modules, hybrid ICs, polycrystalline modules, etc., which have a structure in which components connected to wiring formed on a supporting member by wire bonding, flip-chip bonding, welding, etc. are sealed with an epoxy resin composition; Ball Grid Array (BGA), Chip Size Package (CSP), Multi Chip Package (MCP), etc., which have a structure in which components are mounted on the surface of a supporting member with terminals for wiring board connection formed on the back side, and the components are connected to wiring formed on the supporting member by bumps or wire bonding, and then the components are sealed with an epoxy resin composition. In addition, epoxy resin compositions can also be preferably used in printed wiring boards.

As a method of sealing electronic component devices using epoxy resin compositions, low-pressure transfer molding, injection molding, compression molding, etc. can be listed. Among these, low-pressure transfer molding is generally used. [Example]

The present invention is described in detail below by using embodiments, but the scope of the present invention is not limited to these embodiments.

[Preparation of epoxy resin composition] The following components were pre-mixed (dry mixed) in the proportions shown in Table 1, kneaded for about 5 minutes using a double-shaft roller (roller surface at about 95°C), and then cooled and pulverized to prepare the epoxy resin compositions of the examples and comparative examples.

(A) Epoxy resin ･Biphenyl epoxy resin, Mitsubishi Chemical Co., Ltd., product name "YL6121HA" ･Bisphenol F epoxy resin, Nippon Steel & Sumitomo Metal Chemical Co., Ltd., product name "YDF-8170C" (B) Hardener ･Aryl alkylphenol resin, Air Water Co., Ltd., product name "HE910-09" (C) Hardening accelerator ･Phosphorus hardening accelerator (D) Inorganic filler ･Fused silica (silicon dioxide particles with a volume average particle size of 15 nm) ･Alumina 1 (alumina particles with a volume average particle size of 10.4 μm) ･Alumina 2 (volume average particle size of 2.0 μm alumina particles) ･Alumina 3 (alumina particles with a volume average particle size of 0.40 μm) (E) Fatty acid amide compounds with carbon numbers of 17 to 50 ･Ethylene dioleic acid amide (unsaturated fatty acid amide with carbon number 36)

[Evaluation of the feasibility of mixing] Based on the appearance of the obtained epoxy resin composition, the feasibility of mixing was evaluated according to the following criteria. If the mixing evaluation is A, the dispersibility of the inorganic filler is excellent, so it can be judged that the fluidity of the epoxy resin composition is also good. A: The epoxy resin composition after mixing is not powdery, and the dispersibility of the inorganic filler is excellent. B: The epoxy resin composition after mixing is powdery, and the dispersibility of the inorganic filler is insufficient. In addition, the epoxy resin composition with good mixing evaluation could produce a cured product well, while the epoxy resin composition with poor mixing evaluation could not produce a cured product. It was judged that the poor curing was caused by insufficient dispersion of the curing accelerator.

[Evaluation of thermal conductivity] The thermal conductivity of the epoxy resin composition was evaluated as follows. First, the prepared epoxy resin composition was used to form an epoxy resin composition for thermal conductivity measurement. The epoxy resin composition for thermal conductivity measurement was formed using a vacuum manual press molding machine under the conditions of a mold temperature of 180°C, a molding pressure of 6.9 MPa, and a curing time of 10 minutes. The heat diffusion rate in the thickness direction of the cured product formed into 1 cm×1 cm×0.1 cm by the above method was measured. The heat diffusion rate was measured using a laser flash method (device: LFA467 HyperFlash, NETZSCH Japan Co., Ltd.). Pulse light irradiation was performed under the conditions of pulse width 0.1 (ms) and applied voltage 247 V. The measurement was performed at an ambient temperature of 25℃±1℃. Next, using formula (1), the value of thermal conductivity was obtained by multiplying the heat diffusion rate by the specific heat and density. λ=α×Cp×ρ…Formula (1) (In formula (1), λ represents thermal conductivity (W/(m･K)), α represents heat diffusion rate (m ² /s), Cp represents specific heat (J/(kg･K)), and ρ represents density (d: kg/m ³ ))

[Table 1]

As shown in Table 1, the epoxy resin compositions of Examples 1 and 2 have better thermal conductivity after curing than the epoxy resin composition of Comparative Example 1. Furthermore, in Examples 1 and 2, mixing can be performed even when alumina is highly filled, and an epoxy resin composition for sealing with excellent fluidity can be manufactured. On the other hand, in Comparative Examples 2 and 3, mixing cannot be performed well when alumina is highly filled, and an epoxy resin composition for sealing cannot be manufactured.

The disclosure of Japanese Patent Application No. 2017-209354 filed on October 30, 2017 is incorporated in its entirety into this specification by reference. All documents, patent applications, and technical specifications described in this specification are incorporated in this specification by reference to the same extent as if each document, patent application, and technical specification were specifically and individually described as being incorporated by reference.

without

without

Claims (4)

A sealing epoxy resin composition comprises (A) epoxy resin, (B) hardener, (C) hardening accelerator, (D) inorganic filler and (E) fatty acid amide compound with carbon number of 17 to 50, wherein the inorganic filler (D) comprises aluminum oxide, the content of the aluminum oxide is 83 volume % or more relative to the total amount of the composition, and the content of inorganic fillers other than aluminum oxide in the inorganic filler (D) is 0.1 volume % to 3 volume % relative to the total amount of the inorganic filler (D). As described in item 1 of the patent application, the content of the fatty acid amide compound (E) having 17 to 50 carbon atoms is 0.005% to 1.0% by mass relative to the total amount of the composition. The sealing epoxy resin composition as described in item 1 of the patent application, wherein the (E) fatty acid amide compound having 17 to 50 carbon atoms comprises at least one compound selected from the group consisting of oleamide, stearamide, erucic acid amide, ethylenebisoleamide, hexamethylenebisoleamide, dioleyl adipamide, methylenebiserucic acid amide, ethylenebiserucic acid amide, hexamethylenebiserucic acid amide, meta-xylenebiserucic acid amide, paraphenylenebiserucic acid amide, methylenebisstearic acid amide, and ethylenebislauric acid amide. An electronic component device comprises a component and a cured product of the sealing epoxy resin composition as described in any one of items 1 to 3 of the patent application for sealing the component.