Epoxy resin composition and electronic component device

Abstract

An epoxy resin composition contains an epoxy resin, a curing agent, an inorganic filler, and a silane compound having a structure in which a chain hydrocarbon group having 6 or more carbon atoms is bonded to a silicon atom.

Description

Technical Field

[0001] This disclosure relates to an epoxy resin composition and an electronic component device. Background Technology

[0002] For a long time, resin sealing has been the mainstream method for sealing electronic components such as transistors and integrated circuits (ICs) due to factors such as productivity and cost. Furthermore, in recent years, the high-density mounting of electronic components on printed circuit boards has been advancing. Along with this, semiconductor devices have shifted from through-hole packaging to surface-mount packaging. Surface-mount ICs and LSIs (Large-Scale Integration) have become thin and small packages to improve sealing and reduce mounting height, resulting in a larger component footprint relative to the package and a very thin package wall.

[0003] Furthermore, due to the increasing multifunctionality and capacity of components, chip area is increasing and pin counts are multiplying. Further, by increasing the number of pads (electrodes), the spacing between pads and the size of pads—the so-called narrow pad spacing—is also being reduced. In addition, to cope with further miniaturization and weight reduction, packaging forms are transitioning from QFP (Quad Flat Package) and SOP (Small Outline Package) to CSP (Chip Size Package) and BGA (Ball Grid Array), which are more suitable for multiplying and enable higher density mounting.

[0004] In addition to the commonly used transfer molding method, other methods for sealing electronic components include compression molding (see, for example, Patent Document 1). Compression molding involves supplying a granular resin composition in a manner opposite to the object to be sealed (such as a substrate containing electronic components like semiconductor chips) held within a mold, and compressing the object to be sealed and the granular resin composition to achieve resin sealing.

[0005] With the increasing versatility of packaging, the built-in leads have become thinner, thus making it a challenge to suppress lead misalignment in transfer molding, which is commonly used as a sealing method. On the other hand, even when using compression molding, it is desirable to suppress viscosity from the perspective of filling properties.

[0006] Furthermore, the miniaturization and increasing density of electronic components tend to lead to increased heat generation, making heat dissipation an important issue. Therefore, the integration of inorganic fillers with high thermal conductivity into sealing materials has been explored to improve thermal conductivity.

[0007] When inorganic fillers are mixed into sealants, there are concerns that as the amount of inorganic filler increases, the viscosity of the sealant increases, the fluidity decreases, and problems such as poor filling and lead wire misalignment occur. Therefore, a method to improve the fluidity of sealants by using a specific phosphorus compound as a curing accelerator has been proposed (for example, see Patent Document 2).

[0008] Existing technical documents

[0009] Patent documents

[0010] Patent Document 1: Japanese Patent Application Publication No. 2008-279599

[0011] Patent Document 2: Japanese Patent Application Publication No. 9-157497 Summary of the Invention

[0012] The problem that the invention aims to solve

[0013] However, in conventional methods, there is room for improvement in suppressing the viscosity of the resin composition used as a sealant.

[0014] Furthermore, with the further development of miniaturization and high density of electronic components, it is desirable to provide a resin composition that can be used as a sealant that maintains thermal conductivity at a higher level and suppresses the increase in viscosity.

[0015] In view of the above, the objective of the first embodiment of this disclosure is to provide a low-viscosity epoxy resin composition and an electronic component device having elements sealed by the epoxy resin composition.

[0016] The objective of the second embodiment of this disclosure is to provide an epoxy resin composition having high thermal conductivity and whose viscosity rise is suppressed, and an electronic component device having an element sealed using the epoxy resin composition.

[0017] Methods for solving problems

[0018] The embodiments of this disclosure include the following methods.

[0019] <1> An epoxy resin composition comprising an epoxy resin, a curing agent, an inorganic filler, and a silane compound having a structure in which chain hydrocarbon groups with a carbon number greater than or equal to 6 are bonded to silicon atoms.

[0020] <2> According to the epoxy resin composition of <1>, the above-mentioned chain hydrocarbon group has at least one functional group selected from (meth)acryloyl, epoxy and alkoxy.

[0021] <3> According to the epoxy resin composition described in <1> or <2>, the above-mentioned chain hydrocarbon group has a (meth)acryloyl group.

[0022] <4> In any one of <1> to <3>, the content of the inorganic filler in the epoxy resin composition is 30% to 99% by volume.

[0023] <5> In any one of <1> to <4>, the thermal conductivity of the inorganic filler in the epoxy resin composition is greater than or equal to 20 W / (m·K).

[0024] <6> According to the epoxy resin composition of <5>, the inorganic filler with a thermal conductivity greater than or equal to 20 W / (m·K) comprises at least one selected from the group consisting of alumina, silicon nitride, boron nitride, aluminum nitride, magnesium oxide and silicon carbide.

[0025] <7> An electronic component device comprising an element sealed by any one of <1> to <6> of an epoxy resin composition.

[0026] Invention Effects

[0027] According to a first embodiment of the present disclosure, a low-viscosity epoxy resin composition and an electronic component device having elements sealed by the epoxy resin composition are provided.

[0028] According to a second embodiment of this disclosure, an epoxy resin composition having high thermal conductivity and whose viscosity rise is suppressed is provided, and an electronic component device having an element sealed using the epoxy resin composition. Detailed Implementation

[0029] The following describes in detail the methods for carrying out the present invention. However, the present invention is not limited to the embodiments described below. In the embodiments described below, the constituent elements (including element steps, etc.) are not essential unless specifically stated otherwise. Similarly, numerical values ​​and their ranges are not intended to limit the present invention.

[0030] In this disclosure, the numerical range represented by “~” indicates the range of minimum and maximum values ​​recorded before and after “~”, respectively.

[0031] In the numerical ranges described in this disclosure, the upper or lower limit of one numerical range can be replaced by the upper or lower limit of another numerical range described in other stages. Furthermore, the upper or lower limit of the numerical ranges described in this disclosure can also be replaced by the values ​​shown in the embodiments.

[0032] This disclosure may also include multiple substances equivalent to each component. In the case of multiple substances equivalent to each component present in the composition, unless otherwise specified, the content or percentage of each component refers to the total content or percentage of the multiple substances present in the composition.

[0033] In this disclosure, multiple particles equivalent to each component may also be included. When multiple particles equivalent to each component are present in the composition, unless otherwise specified, the particle size of each component refers to a value for a mixture of the multiple particles present in the composition.

[0034] In this disclosure, the term (meth)acryloyl means at least one of acryloyl and methacryloyl.

[0035] <Epoxy Resin Composition According to Embodiment 1>

[0036] The epoxy resin composition according to the first embodiment contains an epoxy resin, a curing agent, an inorganic filler, and a silane compound having a structure in which chain-like hydrocarbon groups with 6 or more carbon atoms are bonded to silicon atoms. It should be noted that, in this disclosure, silane compounds having a structure in which chain-like hydrocarbon groups with 6 or more carbon atoms are bonded to silicon atoms are also referred to as "specific silane compounds." The epoxy resin composition according to the first embodiment may also contain other components as needed.

[0037] If the epoxy resin composition has the above-described structure, a low-viscosity epoxy resin composition can be obtained. While the detailed reasons for the low viscosity of the epoxy resin composition with the above-described structure may not be clear, they can be inferred as follows: Generally, to improve the dispersibility of inorganic fillers, low-molecular-weight coupling agents such as propyl-containing silane compounds can be used in sealing resin compositions. In contrast, if a silane compound with a longer-chain hydrocarbon group is used, it is believed that the compatibility of the inorganic filler with the resin is improved, and the frictional resistance between the inorganic fillers is reduced. As a result, it is inferred that the melt viscosity decreases compared to the case where a low-molecular-weight coupling agent is used instead of a specific silane compound. Furthermore, it is inferred that by using a low-viscosity epoxy resin composition, it is possible to obtain components with suppressed lead wire deflection and electronic component devices incorporating such components.

[0038] Hereinafter, the components of the epoxy resin composition according to the first embodiment will be described in detail.

[0039] (Epoxy resin)

[0040] The epoxy resin composition according to the first embodiment contains an epoxy resin. There are no particular limitations on the type of epoxy resin, as long as it has epoxy groups in its molecule.

[0041] Specifically, examples of epoxy resins include: epoxidation of phenolic varnish resins obtained by condensing or co-condensing phenolic compounds selected from the group consisting of phenol, cresol, xylenol, resorcinol, catechol, bisphenol A, bisphenol F, and naphthol compounds such as α-naphthol, β-naphthol, and dihydroxynaphthol with aliphatic aldehyde compounds such as formaldehyde, acetaldehyde, and propionaldehyde under an acidic catalyst to obtain phenolic varnish epoxy resins (phenolic varnish epoxy resins, o-cresol varnish epoxy resins, etc.); epoxidation of the above-mentioned phenolic... Triphenylmethane-type epoxy resin obtained by epoxidation of triphenylmethane-type phenolic resin obtained by condensing or co-condensing the compound with aromatic aldehyde compounds such as benzaldehyde and salicylaldehyde under an acidic catalyst; copolymer epoxy resin obtained by epoxidation of phenolic varnish resin obtained by co-condensing the above-mentioned phenolic compound and naphthol compound with aldehyde compound under an acidic catalyst; diphenylmethane-type epoxy resin as diglycidyl ether of bisphenol A, bisphenol F, etc.; biphenyl-type epoxy resin as diglycidyl ether of alkyl-substituted or unsubstituted biphenyl phenol; as... diglycidyl ether of phenolic compounds Epoxy resins of various types; epoxy resins containing sulfur atoms as diglycidyl ethers of bisphenol S, etc.; epoxy resins as glycidyl ethers of alcohols such as butanediol, polyethylene glycol, and polypropylene glycol; glycidyl ester type epoxy resins as glycidyl esters of polycarboxylic acid compounds such as phthalic acid, isophthalic acid, and tetrahydrophthalic acid; glycidylamine type epoxy resins obtained by replacing the active hydrogen atom of nitrogen atoms of aniline, diaminodiphenylmethane, isocyanuric acid, etc. with glycidyl groups; dicyclopentadiene type epoxy resins obtained by epoxidizing a co-condensation resin of dicyclopentadiene and phenolic compounds; vinylcyclohexene diepoxide, 3,4-epoxycyclohexylmethyl-3,4-epoxycyclohexane carboxylate, and 2-(3,4-epoxy)cyclohexyl-5,5-spirocyclo(3,4-epoxy)cyclohexane-m-dicyclohexane obtained by epoxidizing the olefin bonds within the molecule. Alicyclic epoxy resins such as alkylene oxides; p-xylene-modified epoxy resins as glycidyl ethers of p-xylene-modified phenolic resins; m-xylene-modified epoxy resins as glycidyl ethers of m-xylene-modified phenolic resins; terpene-modified epoxy resins as glycidyl ethers of terpene-modified phenolic resins; dicyclopentadiene-modified epoxy resins as glycidyl ethers of dicyclopentadiene-modified phenolic resins; cyclopentadiene-modified epoxy resins as glycidyl ethers of cyclopentadiene-modified phenolic resins; as multi-... Polycyclic aromatic ring modified epoxy resins are derived from glycidyl ethers of cyclic aromatic ring modified phenolic resins; naphthalene-type epoxy resins are derived from glycidyl ethers of naphthalene-containing phenolic resins; halogenated phenolic varnish-type epoxy resins; hydroquinone-type epoxy resins; trimethylolpropane-type epoxy resins; linear aliphatic epoxy resins obtained by oxidizing olefin bonds using peracetic acids such as peracetic acid; and aralkyl-type epoxy resins obtained by epoxidizing aralkyl-type phenolic resins such as phenol aralkyl resins and naphthol aralkyl resins. Furthermore, epoxides of organosilicon resins and epoxides of acrylic resins can also be used as epoxy resins. These epoxy resins can be used alone or in combination of two or more.

[0042] There are no particular limitations on the epoxy equivalent (molecular weight / number of epoxy groups) of the epoxy resin. From the viewpoint of balancing various properties such as moldability, reflow solderability and electrical reliability, it is preferred to be 100 g / eq to 1000 g / eq, and more preferably 150 g / eq to 500 g / eq.

[0043] The epoxy equivalent of the epoxy resin is set as a value determined by means of the method according to JIS K 7236:2009.

[0044] When the epoxy resin is a solid, its softening point or melting point is not particularly limited. From the viewpoint of moldability and reflow solderability, 40°C to 180°C is preferred, and from the viewpoint of operability when preparing the epoxy resin composition, 50°C to 130°C is more preferred.

[0045] The melting point of the epoxy resin is set as the value determined by differential scanning calorimetry (DSC), and the softening point of the epoxy resin is set as the value determined by the method (ring and ball method) according to JIS K 7234:1986.

[0046] From the viewpoints of strength, flowability, heat resistance, and moldability, the content of epoxy resin in the epoxy resin composition is preferably 0.5% to 50% by mass, more preferably 2% to 30% by mass, and even more preferably 2% to 20% by mass.

[0047] (Curing agent)

[0048] The epoxy resin composition according to the first embodiment contains a curing agent. There are no particular limitations on the type of curing agent; it can be selected based on the type of resin, the desired properties of the epoxy resin composition, etc.

[0049] Examples of curing agents include phenolic curing agents, amine curing agents, acid anhydride curing agents, polythiol curing agents, polyaminoamide curing agents, isocyanate curing agents, and end-capped isocyanate curing agents. From the viewpoint of improving heat resistance, curing agents preferably have phenolic hydroxyl groups in their molecules (phenolic curing agents).

[0050] Specifically, examples of phenolic curing agents include: resorcinol, catechol, bisphenol A, bisphenol F, substituted or unsubstituted biphenols, and other polyphenolic compounds; phenolic varnish-type phenolic resins obtained by condensing or co-condensing at least one phenolic compound selected from the group consisting of phenol, cresol, xylenol, resorcinol, catechol, bisphenol A, bisphenol F, phenylphenol, aminophenol, and naphthol compounds such as α-naphthol, β-naphthol, and dihydroxynaphthol with aldehyde compounds such as formaldehyde, acetaldehyde, propionaldehyde, benzaldehyde, and salicylaldehyde under an acidic catalyst; and phenolic varnish-type phenolic resins synthesized from the above phenolic compounds and dimethoxy-p-xylene, bis(methoxymethyl)biphenyl, etc. Aryl alkyl phenolic resins such as phenol and naphthol aryl alkyl resins; p-xylene and / or m-xylene modified phenolic resins; melamine modified phenolic resins; terpene modified phenolic resins; dicyclopentadiene-type phenolic resins and dicyclopentadiene-type naphthol-type phenolic resins synthesized by copolymerization of the above phenolic compounds with dicyclopentadiene; cyclopentadiene modified phenolic resins; polycyclic aromatic ring modified phenolic resins; biphenyl-type phenolic resins; triphenylmethane-type phenolic resins obtained by condensing or co-condensing the above phenolic compounds with aromatic aldehydes such as benzaldehyde and salicylaldehyde under an acidic catalyst; and phenolic resins obtained by copolymerizing two or more of these. These phenolic curing agents can be used alone or in combination of two or more.

[0051] There are no particular limitations on the functional group equivalent of the curing agent (hydroxyl equivalent in the case of phenolic curing agents). From the viewpoint of balancing various properties such as moldability, reflow resistance, and electrical reliability, 70 g / eq to 1000 g / eq is preferred, and 80 g / eq to 500 g / eq is more preferred.

[0052] The functional group equivalent of the curing agent (hydroxyl equivalent in the case of phenolic curing agents) is set as a value determined by the method according to JIS K0070:1992.

[0053] When the curing agent is a solid, its softening point or melting point is not particularly limited. From the viewpoint of moldability and reflow solderability, 40°C to 180°C is preferred, and from the viewpoint of operability in the manufacture of epoxy resin compositions, 50°C to 130°C is more preferred.

[0054] The melting point or softening point of the curing agent is set to the same value as that of the epoxy resin, which was measured in the same way.

[0055] The equivalent ratio of epoxy resin to curing agent, i.e., the ratio of the number of functional groups in the curing agent to the number of epoxy groups in the epoxy resin (number of functional groups in the curing agent / number of epoxy groups in the epoxy resin), is not particularly limited. From the perspective of minimizing unreacted components, a range of 0.5 to 2.0 is preferred, and a range of 0.6 to 1.3 is more preferable. From the viewpoint of moldability and reflow resistance, a range of 0.8 to 1.2 is further preferred.

[0056] (Inorganic filler material)

[0057] The epoxy resin composition according to the first embodiment contains an inorganic filler. There are no particular limitations on the material of the inorganic filler.

[0058] Inorganic filler materials can include, specifically: fused silica, crystalline silica, glass, alumina, calcium carbonate, zirconium silicate, calcium silicate, silicon nitride, aluminum nitride, boron nitride, magnesium oxide, silicon carbide, beryllium oxide, zircon, zircon, forsterite, blocky talc, spinel, mullite, titanium dioxide, talc, clay, mica, and other inorganic materials. Inorganic fillers with flame-retardant properties can also be used. Examples of flame-retardant inorganic fillers include aluminum hydroxide, magnesium hydroxide, composite metal hydroxides such as magnesium and zinc hydroxides, and zinc borate.

[0059] Among inorganic fillers, from the viewpoint of reducing the coefficient of linear expansion, fused silica and other silica are preferred, while from the viewpoint of high thermal conductivity, alumina is preferred.

[0060] There are no particular restrictions on the shape of inorganic fillers, but spherical shapes are preferred from the perspectives of filling performance and mold abrasion resistance.

[0061] Inorganic fillers can be used alone or in combination with two or more. It should be noted that "combining two or more inorganic fillers" can include, for example, the use of two or more inorganic fillers with the same composition but different average particle sizes; the use of two or more inorganic fillers with the same average particle size but different compositions; and the use of two or more inorganic fillers with different average particle sizes and types.

[0062] The content of inorganic filler in the epoxy resin composition according to the first embodiment is not particularly limited. From the viewpoint of further improving the properties of the cured product, such as the coefficient of thermal expansion, thermal conductivity, and modulus of elasticity, the content of inorganic filler is preferably greater than or equal to 30% by volume of the total epoxy resin composition, more preferably greater than or equal to 35% by volume, even more preferably greater than or equal to 40% by volume, particularly preferably greater than or equal to 45% by volume, and extremely preferably greater than or equal to 50% by volume. From the viewpoint of improving fluidity and reducing viscosity, the content of inorganic filler is preferably less than or equal to 99% by volume of the total epoxy resin composition, preferably less than or equal to 98% by volume, and more preferably less than or equal to 97% by volume.

[0063] In addition, for example, when the epoxy resin composition is used for compression molding, the content of inorganic filler can be set to 70% to 99% of the total epoxy resin composition, or 80% to 99% of the total epoxy resin composition, or 83% to 99% of the total epoxy resin composition, or 85% to 99% of the total epoxy resin composition.

[0064] The content of inorganic fillers in the epoxy resin composition was determined as follows. First, the total mass of the cured epoxy resin composition (epoxy resin molded article) was measured. This epoxy resin molded article was then fired at 400°C for 2 hours, followed by firing at 700°C for 3 hours to evaporate the resin components. The mass of the remaining inorganic fillers was measured. Based on the obtained masses and their respective specific gravities, the volume was calculated, and the ratio of the volume of the inorganic fillers to the total volume of the epoxy resin molded article was taken as the content of the inorganic fillers.

[0065] When the inorganic filler is in particulate form, its average particle size is not particularly limited. For example, the overall volume average particle size of the inorganic filler is preferably less than or equal to 80 μm, but can also be less than or equal to 50 μm, 40 μm, 30 μm, 25 μm, 20 μm, or 15 μm. Furthermore, the overall volume average particle size of the inorganic filler is preferably greater than or equal to 0.1 μm, more preferably greater than or equal to 0.2 μm, and even more preferably greater than or equal to 0.3 μm. If the volume average particle size of the inorganic filler is greater than or equal to 0.1 μm, there is a tendency for the viscosity increase of the epoxy resin composition to be further suppressed. If the volume average particle size is less than or equal to 80 μm, there is a tendency for the filling performance of narrow gaps to be further improved. The volume average particle size of inorganic fillers can be determined as the particle size (D50) when the cumulative particle size distribution from the small diameter side becomes 50% in the volume reference particle size distribution measured by a laser scattering diffraction particle size distribution measuring device.

[0066] In applications such as using epoxy resin compositions for underfilling in molding, from the viewpoint of improving filling performance in narrow gaps, it is preferable that the maximum particle size (cutpoint) of the inorganic filler is controlled. The maximum particle size of the inorganic filler can be appropriately adjusted; from the viewpoint of filling performance, it is preferably less than or equal to 105 μm, more preferably less than or equal to 75 μm, and may also be less than or equal to 60 μm, or even less than or equal to 40 μm. The maximum particle size can be measured using a laser diffraction particle size analyzer (manufactured by Horiba Manufacturing Co., Ltd., trade name: LA920).

[0067] (Specific silane compounds)

[0068] The epoxy resin composition according to the first embodiment contains a specific silane compound. The specific silane compound has a structure formed by combining a chain hydrocarbon group with 6 or more carbon atoms (hereinafter, a chain hydrocarbon group with 6 or more carbon atoms is also simply referred to as a chain hydrocarbon group) with silicon atoms. The chain hydrocarbon group may be branched or may have substituents. It should be noted that, in this disclosure, the number of carbon atoms in the chain hydrocarbon group refers to the number of carbon atoms without branches or substituents. The chain hydrocarbon group may or may not contain unsaturated bonds, but preferably does not contain unsaturated bonds.

[0069] It is believed that certain silane compounds function as coupling agents for inorganic fillers in epoxy resin compositions.

[0070] The number of chain hydrocarbon groups bonded to silicon atoms in a specific silane compound can be 1 to 4, preferably 1 to 3, more preferably 1 or 2, and even more preferably 1.

[0071] When the number of chain hydrocarbon groups bonded to silicon atoms in a specific silane compound is 1 to 3, there are no particular restrictions on the atoms or groups of atoms bonded to silicon atoms other than the chain hydrocarbon groups, and they can be hydrogen atoms, alkyl groups with 1 to 5 carbon atoms, alkoxy groups, aryl groups, aryloxy groups, etc. Preferably, in addition to the chain hydrocarbon groups, one or more alkoxy groups are bonded to the silicon atom, and more preferably, one chain hydrocarbon group and three alkoxy groups are bonded to the silicon atom.

[0072] The chain hydrocarbon group of a particular silane compound has 6 or more carbon atoms, and from the viewpoint of suppressing viscosity, it is preferable to have 7 or more carbon atoms, and more preferably 8 or more carbon atoms. There is no particular upper limit to the number of carbon atoms in the chain hydrocarbon group of a particular silane compound, but from the viewpoint of dispersibility in resin and the balance of physical properties of cured product, it is preferable to have 12 or more carbon atoms, more preferably 11 or more carbon atoms, and even more preferably 10 or more carbon atoms.

[0073] When a chain hydrocarbon group has substituents, the substituents are not particularly limited. Substituents can be present at the end of the chain hydrocarbon group or on the side chain of the chain hydrocarbon group.

[0074] The chain hydrocarbon group preferably has at least one functional group selected from (meth)acryloyl, epoxy, and alkoxy (hereinafter also referred to as a specific functional group), more preferably has at least one functional group selected from (meth)acryloyl and epoxy, and even more preferably has a (meth)acryloyl group. The specific functional group may be present at the end of the chain hydrocarbon group or in the side chain of the chain hydrocarbon group. From the viewpoint of suppressing viscosity, the specific functional group is preferably present at the end of the chain hydrocarbon group.

[0075] If the chain hydrocarbon groups in a particular silane compound possess specific functional groups, there is a tendency for the viscosity of the epoxy resin composition to decrease further. While the reason may not be clear, it is speculated that when the chain hydrocarbon groups in a particular silane compound possess specific functional groups, the compatibility of these functional groups with the epoxy resin increases, and the dispersibility of the epoxy resin with inorganic fillers improves.

[0076] When the chain hydrocarbon group has a (meth)acryloyl group, the (meth)acryloyl group can be directly bonded to the chain hydrocarbon group or bonded through other atoms or groups. For example, the chain hydrocarbon group can also have a (meth)acryloyloxy group. Preferably, the chain hydrocarbon group has a methacryloyloxy group.

[0077] When the chain hydrocarbon group has an epoxy group, the epoxy group can be directly bonded to the chain hydrocarbon group or bonded through other atoms or groups. For example, the chain hydrocarbon group can also have glycidyloxy groups, alicyclic epoxy groups, etc. Among them, the chain hydrocarbon group preferably has a glycidyloxy group.

[0078] When the chain hydrocarbon group has an alkoxy group, the alkoxy group can be directly bonded to the chain hydrocarbon group or bonded through other atoms or groups of atoms; it is preferred that it be directly bonded to the chain hydrocarbon group. The alkoxy group is not particularly limited and can be methoxy, ethoxy, propoxy, isopropoxy, etc. From the viewpoint of ease of acquisition, the chain hydrocarbon group preferably has a methoxy group.

[0079] There is no particular limitation on the equivalent (molecular weight / number of functional groups) of at least one functional group selected from (meth)acryloyl, epoxy, and alkoxy in a specific silane compound. From the viewpoint of reducing the viscosity of the epoxy resin composition, 200 g / eq to 420 g / eq is preferred, more preferably 210 g / eq to 405 g / eq, and even more preferably 230 g / eq to 390 g / eq.

[0080] Examples of specific silane compounds include: hexyltrimethoxysilane, heptyltrimethoxysilane, octyltrimethoxysilane, hexyltriethoxysilane, heptyltriethoxysilane, octyltriethoxysilane, 6-glycidoxyhexyltrimethoxysilane, 7-glycidoxyheptyltrimethoxysilane, 8-glycidoxyoctyltrimethoxysilane, 6-(meth)acryloyloxyhexyltrimethoxysilane, 7-(meth)acryloyloxyheptyltrimethoxysilane, 8-(meth)acryloyloxyoctyltrimethoxysilane, and decyltrimethoxysilane. Among these, 8-glycidoxyoctyltrimethoxysilane and 8-methacryloyloxyoctyltrimethoxysilane are preferred from the viewpoint of reducing the viscosity of the epoxy resin composition. A single specific silane compound may be used, or two or more may be used in combination.

[0081] Certain silane compounds can be synthesized or commercially available silane compounds can be used. Examples of commercially available silane compounds include KBM-3063 (hexyltrimethoxysilane), KBE-3063 (hexyltriethoxysilane), KBE-3083 (octyltriethoxysilane), KBM-4803 (8-glycidoxyoctyltrimethoxysilane), KBM-5803 (8-methacryloyloxyoctyltrimethoxysilane), and KBM-3103C (decyltrimethoxysilane), all manufactured by Shin-Etsu Chemical Co., Ltd.

[0082] The content of the specific silane compound in the epoxy resin composition according to the first embodiment is not particularly limited. The content of the specific silane compound relative to 100 parts by weight of the inorganic filler can be greater than or equal to 0.01 parts by weight, or greater than or equal to 0.02 parts by weight. Furthermore, the content of the specific silane compound relative to 100 parts by weight of the inorganic filler is preferably less than or equal to 5 parts by weight, more preferably less than or equal to 2.5 parts by weight. If the content of the specific silane compound relative to 100 parts by weight of the inorganic filler is greater than or equal to 0.01 parts by weight, there is a tendency to obtain a composition with low viscosity. If the content of the specific silane compound relative to 100 parts by weight of the inorganic filler is less than or equal to 5 parts by weight, there is a tendency to further improve the moldability of the encapsulation.

[0083] (Other coupling agents)

[0084] The epoxy resin composition according to the first embodiment may further contain other coupling agents in addition to the specific silane compound. There are no particular limitations on the other coupling agents, as long as they are coupling agents commonly used in epoxy resin compositions. Examples of other coupling agents include silane compounds (excluding the specific silane compound) such as epoxy silanes, mercaptosilanes, aminosilanes, alkylsilanes, ureosilanes, and vinylsilanes, as well as titanium compounds, aluminum chelate compounds, and aluminum / zirconium compounds. Other coupling agents may be used alone or in combination of two or more.

[0085] When the epoxy resin composition according to the first embodiment contains coupling agents other than a specific silane compound, the total content of the specific silane compound and other coupling agents relative to 100 parts by weight of the inorganic filler can be greater than or equal to 0.01 parts by weight, or greater than or equal to 0.02 parts by weight. Furthermore, the total content of the specific silane compound and other coupling agents relative to 100 parts by weight of the inorganic filler is preferably less than or equal to 5 parts by weight, more preferably less than or equal to 2.5 parts by weight. If the total content of the specific silane compound and other coupling agents relative to 100 parts by weight of the inorganic filler is greater than or equal to 0.01 parts by weight, there is a tendency to obtain a composition with low viscosity. If the total content of the specific silane compound and other coupling agents relative to 100 parts by weight of the inorganic filler is less than or equal to 5 parts by weight, there is a tendency to further improve the moldability of the encapsulation.

[0086] In the case where the epoxy resin composition according to the first embodiment contains coupling agents other than a specific silane compound, from the viewpoint of effectively utilizing the specific silane compound, the content of the other coupling agents is preferably less than or equal to 90% by mass, more preferably less than or equal to 70% by mass, and even more preferably less than or equal to 50% by mass relative to the total amount of the specific silane compound and the other coupling agents.

[0087] (Curing accelerator)

[0088] The epoxy resin composition according to the first embodiment may also contain a curing accelerator. There are no particular limitations on the type of curing accelerator; it can be selected based on the type of epoxy resin, the desired properties of the epoxy resin composition, etc.

[0089] Examples of curing accelerators include: 1,5-diazabicyclo[4.3.0]nonene-5 (DBN), 1,8-diazabicyclo[5.4.0]undecene-7 (DBU), and other diazabicycloolefins; cyclic amidine compounds such as 2-methylimidazole, 2-phenylimidazole, 2-phenyl-4-methylimidazole, and 2-heptadecylimidazole; derivatives of the above cyclic amidine compounds; phenolic varnish salts of the above cyclic amidine compounds or their derivatives; and compounds that have undergone addition reactions with maleic anhydride, 1,4-benzoquinone, and 2... Compounds with intramolecular polarization, such as quinones like 5-toluenequinone, 1,4-naphthoquinone, 2,3-dimethylbenzoquinone, 2,6-dimethylbenzoquinone, 2,3-dimethoxy-5-methyl-1,4-benzoquinone, 2,3-dimethoxy-1,4-benzoquinone, and phenyl-1,4-benzoquinone, and compounds with π bonds like diazonylmethane; cyclic amidines such as tetraphenylborate of DBU, tetraphenylborate of DBN, tetraphenylborate of 2-ethyl-4-methylimidazolium, and tetraphenylborate of N-methylmorpholine. Compounds; tertiary amine compounds such as pyridine, triethylamine, triethylenediamine, benzyldimethylamine, triethanolamine, dimethylaminoethanol, and tris(dimethylaminomethyl)phenol; derivatives of the above tertiary amine compounds; ammonium salts such as tetrabutylammonium acetate, tetrabutylammonium phosphate, tetraethylammonium acetate, tetrahexylammonium benzoate, and tetrapropylammonium hydroxide; triphenylphosphine, diphenyl(p-tolyl)phosphine, tris(alkylphenyl)phosphine, tris(alkoxyphenyl)phosphine, and tris(alkyl-alkyl)phosphine. Phosphine compounds including tertiary phosphines such as tri(dialkylphenyl)phosphine, tri(trialkylphenyl)phosphine, tri(tetraalkylphenyl)phosphine, tri(dialkoxyphenyl)phosphine, tri(trialkoxyphenyl)phosphine, tri(tetraalkoxyphenyl)phosphine, trialkylphosphine, dialkylarylphosphine, and alkyldiarylphosphine; phosphine compounds such as complexes of the above tertiary phosphines with organoboron compounds; and phosphine compounds containing maleic anhydride, 1,4-benzoquinone, 2,5-toluenequinone, 1,4-naphthoquinone, and 2,3- Compounds with intramolecular polarization formed by the addition of quinone compounds such as dimethylbenzoquinone, 2,6-dimethylbenzoquinone, 2,3-dimethoxy-5-methyl-1,4-benzoquinone, 2,3-dimethoxy-1,4-benzoquinone, and phenyl-1,4-benzoquinone, and compounds with π bonds such as diazophenylmethane; tertiary phosphine or the above-mentioned phosphine compounds with 4-bromophenol, 3-bromophenol, 2-bromophenol, 4-chlorophenol, 3-chlorophenol, 2-chlorophenol, or 4-iodophenol. Compounds with intramolecular polarization obtained by reacting halogenated phenolic compounds such as 3-iodophenol, 2-iodophenol, 4-bromo-2-methylphenol, 4-bromo-3-methylphenol, 4-bromo-2,6-dimethylphenol, 4-bromo-3,5-dimethylphenol, 4-bromo-2,6-di-tert-butylphenol, 4-chloro-1-naphthol, 1-bromo-2-naphthol, 6-bromo-2-naphthol, and 4-bromo-4'-hydroxybiphenyl with hydrogen halide; tetraphenyl Quadrilateral replacement Tetra-p-tolylborates and similar products do not contain tetrasubstituted phenyl groups bonded to boron atoms. and tetrasubstituted borates; tetraphenyl Salts of phenolic compounds, etc. Curing accelerators can be used alone or in combination of two or more.

[0090] When the epoxy resin composition according to the first embodiment contains a curing accelerator, the amount of the curing accelerator is preferably 0.1 to 30 parts by mass relative to 100 parts by mass of the resin component (i.e., the total of the resin and the curing agent), more preferably 1 to 15 parts by mass. If the amount of the curing accelerator is greater than or equal to 0.1 parts by mass relative to 100 parts by mass of the resin component, there is a tendency for good curing in a short time. If the amount of the curing accelerator is less than or equal to 30 parts by mass relative to 100 parts by mass of the resin component, there is a tendency for a good molded article to be obtained without the curing speed being too fast.

[0091] [Various additives]

[0092] In addition to the components described above, the epoxy resin composition according to the first embodiment may also contain various additives such as ion exchangers, release agents, flame retardants, colorants, and stress relievers, as exemplified below. The epoxy resin composition according to the first embodiment may also contain various additives well-known in the art, in addition to the additives exemplified below, as needed.

[0093] (ion exchanger)

[0094] The epoxy resin composition according to the first embodiment may also contain an ion exchanger. Particularly when using the epoxy resin composition according to the first embodiment as a sealing molding material, from the viewpoint of improving the moisture resistance and high-temperature storage characteristics of the electronic component device with the element to be sealed, the presence of an ion exchanger is preferred. There are no particular limitations on the ion exchanger; conventionally known ion exchangers can be used. Specifically, examples include hydrotalcite compounds and hydrated oxides of at least one element selected from the group consisting of magnesium, aluminum, titanium, zirconium, and bismuth. One ion exchanger may be used alone, or two or more may be used in combination. Hydrotalcite represented by the following general formula (A) is preferred.

[0095] Mg (1-X) Al X (OH)2(CO3) X / 2 ·mH2O……(A)

[0096] (0 < X ​​≤ 0.5, m is a positive number)

[0097] When the epoxy resin composition according to the first embodiment contains an ion exchanger, its content is not particularly limited as long as it is sufficient to capture halogen ions and other ions. For example, it is preferably 0.1 to 30 parts by mass relative to 100 parts by mass of resin components, and more preferably 1 to 10 parts by mass.

[0098] (Mold release agent)

[0099] From the viewpoint of achieving good release properties from the mold during molding, the epoxy resin composition according to the first embodiment may also contain a release agent. There are no particular limitations on the release agent, and conventionally known release agents can be used. Specifically, examples include: carnauba wax, higher fatty acids such as linalool and stearic acid, metal salts of higher fatty acids, ester waxes such as linalool esters, polyolefin waxes such as oxidized polyethylene and non-oxidized polyethylene, etc. A single release agent may be used, or two or more may be used in combination.

[0100] When the epoxy resin composition according to the first embodiment contains a release agent, the amount of release agent is preferably 0.01 to 10 parts by weight, more preferably 0.1 to 5 parts by weight, relative to 100 parts by weight of the resin component. If the amount of release agent is greater than or equal to 0.01 parts by weight relative to 100 parts by weight of the resin component, there is a tendency to obtain sufficient release properties. If it is less than or equal to 10 parts by weight, there is a tendency to obtain better adhesion and curing properties.

[0101] (Flame retardant)

[0102] The epoxy resin composition according to the first embodiment may also contain a flame retardant. There are no particular limitations on the flame retardant; conventionally known flame retardants can be used. Specifically, examples include organic or inorganic compounds containing halogen atoms, antimony atoms, nitrogen atoms, or phosphorus atoms, metal hydroxides, etc. A single flame retardant may be used, or two or more may be used in combination.

[0103] When the epoxy resin composition according to the first embodiment contains a flame retardant, there is no particular limitation on the amount of flame retardant, as long as it is sufficient to obtain the desired flame retardant effect. For example, it is preferably 1 to 30 parts by weight, and more preferably 2 to 20 parts by weight, relative to 100 parts by weight of the resin component.

[0104] (Coloring agent)

[0105] The epoxy resin composition according to the first embodiment may further contain a colorant. Examples of known colorants include carbon black, organic dyes, organic pigments, titanium dioxide, red lead, and iron oxide. The content of the colorant can be appropriately selected according to the purpose, etc. A single colorant may be used, or two or more may be used in combination.

[0106] (Stress reliever)

[0107] The epoxy resin composition according to the first embodiment may also contain stress-relieving agents such as silicone oil and silicone rubber particles. By containing stress-relieving agents, it is possible to further reduce the warpage and cracking of the encapsulation. Commonly used and known stress-relieving agents (flexible agents) can be listed as stress-relieving agents. Specifically, examples include: thermoplastic elastomers such as organosilicon, styrene, olefin, urethane, polyester, polyether, polyamide, and polybutadiene; NR (natural rubber); NBR (acrylonitrile-butadiene rubber); acrylic rubber; urethane rubber; rubber particles such as organosilicon powder; and rubber particles with a core-shell structure such as methyl methacrylate-styrene-butadiene copolymer (MBS), methyl methacrylate-organosilicon copolymer, and methyl methacrylate-butyl acrylate copolymer. Stress-relieving agents can be used alone or in combination of two or more.

[0108] <Epoxy Resin Composition According to Embodiment 2>

[0109] The epoxy resin composition according to the second embodiment contains: epoxy resin, curing agent, inorganic filler with a thermal conductivity greater than or equal to 20 W / (m·K), and a silane compound (specific silane compound) having a structure in which chain hydrocarbon groups with a carbon atom number greater than or equal to 6 are bonded to silicon atoms. It should be noted that the thermal conductivity of the inorganic filler in this disclosure is set to the thermal conductivity at room temperature (25°C). The epoxy resin composition according to the second embodiment may also contain other components as needed.

[0110] With the above configuration, an epoxy resin composition exhibiting high thermal conductivity and suppressed viscosity rise can be obtained. While the detailed reasons for the above-mentioned effects of the epoxy resin composition according to the second embodiment may not be clear, they can be inferred as follows.

[0111] Typically, in sealing resin compositions, low-molecular-weight coupling agents such as propyl silane compounds are used to improve the dispersibility of inorganic fillers. It is believed that using silane compounds with longer-chain hydrocarbon groups improves the compatibility of the inorganic filler with the resin and reduces the frictional resistance between the inorganic fillers. As a result, it is speculated that the melt viscosity decreases compared to using low-molecular-weight coupling agents without specific silane compounds. Therefore, it is hypothesized that by increasing the amount of highly thermally conductive inorganic fillers while suppressing viscosity increases, higher thermal conductivity can be achieved compared to previous methods.

[0112] Hereinafter, the components of the epoxy resin composition according to the second embodiment will be described in detail.

[0113] (Epoxy resin)

[0114] The epoxy resin composition according to the second embodiment contains epoxy resin. Details of the epoxy resin are the same as those of the epoxy resin used in the epoxy resin composition according to the first embodiment.

[0115] (Curing agent)

[0116] The epoxy resin composition according to the second embodiment contains a curing agent. The details of the curing agent are the same as those of the curing agent used in the epoxy resin composition according to the first embodiment.

[0117] (Inorganic filler material)

[0118] The epoxy resin composition according to the second embodiment contains an inorganic filler with a thermal conductivity greater than or equal to 20 W / (m·K). The material of the inorganic filler is not particularly limited as long as it has the above-mentioned thermal conductivity.

[0119] In this disclosure, an inorganic filler with a thermal conductivity greater than or equal to 20 W / (m·K) refers to an inorganic filler composed of a material with a thermal conductivity greater than or equal to 20 W / (m·K) at room temperature (25°C). The thermal conductivity of the inorganic filler can be obtained by measuring the thermal conductivity of the material constituting the inorganic filler using the xenon-flash method or the hot-wire method.

[0120] The thermal conductivity of the inorganic filler is greater than or equal to 20 W / (m·K), and from the viewpoint of heat dissipation when the product is cured, it is preferably greater than or equal to 25 W / (m·K). There is no particular upper limit to the thermal conductivity of the inorganic filler; it can be less than or equal to 500 W / (m·K) or less than or equal to 300 W / (m·K).

[0121] Inorganic filler materials with the aforementioned thermal conductivity include, specifically, alumina, silicon nitride, boron nitride, aluminum nitride, magnesium oxide, and silicon carbide. Among these, alumina is preferred due to its high sphericity and moisture resistance.

[0122] There are no particular restrictions on the shape of inorganic fillers, but spherical shapes are preferred from the perspectives of filling performance and mold abrasion resistance.

[0123] Inorganic fillers can be used alone or in combination with two or more. It should be noted that "combining two or more inorganic fillers" can include, for example, the use of two or more inorganic fillers with the same composition but different average particle sizes; the use of two or more inorganic fillers with the same average particle size but different compositions; and the use of two or more inorganic fillers with different average particle sizes and types.

[0124] The content of inorganic filler in the epoxy resin composition according to the second embodiment is not particularly limited. From the viewpoint of further improving the properties of the cured product, such as the coefficient of thermal expansion, thermal conductivity, and modulus of elasticity, the content of inorganic filler is preferably greater than or equal to 30% by volume of the total epoxy resin composition, more preferably greater than or equal to 35% by volume, even more preferably greater than or equal to 40% by volume, particularly preferably greater than or equal to 45% by volume, and extremely preferably greater than or equal to 50% by volume. From the viewpoint of improving fluidity and reducing viscosity, the content of inorganic filler is preferably less than or equal to 99% by volume of the total epoxy resin composition, preferably less than or equal to 98% by volume, and more preferably less than or equal to 97% by volume.

[0125] The inorganic filler content in the epoxy resin composition according to the second embodiment is preferably 30 vol% to 99 vol%, more preferably 35 vol% to 99 vol%, further preferably 40 vol% to 98 vol%, particularly preferably 45 vol% to 97 vol%, and extremely preferably 50 vol% to 97 vol%.

[0126] The content of inorganic fillers in the epoxy resin composition was determined as follows. First, the total mass of the cured epoxy resin composition (epoxy resin molded article) was measured. This epoxy resin molded article was then fired at 400°C for 2 hours, followed by firing at 700°C for 3 hours to evaporate the resin components. The mass of the remaining inorganic fillers was measured. Based on the obtained masses and their respective specific gravities, the volume was calculated, and the ratio of the volume of the inorganic fillers to the total volume of the epoxy resin molded article was taken as the content of the inorganic fillers.

[0127] When the inorganic filler is in particulate form, its average particle size is not particularly limited. For example, the overall volume average particle size of the inorganic filler is preferably less than or equal to 80 μm, but can also be less than or equal to 50 μm, 40 μm, 30 μm, 25 μm, 20 μm, or 15 μm. Furthermore, the overall volume average particle size of the inorganic filler is preferably greater than or equal to 0.1 μm, more preferably greater than or equal to 0.2 μm, and even more preferably greater than or equal to 0.3 μm. If the volume average particle size of the inorganic filler is greater than or equal to 0.1 μm, there is a tendency for the viscosity increase of the epoxy resin composition to be further suppressed. If the volume average particle size is less than or equal to 80 μm, there is a tendency for the filling performance of narrow gaps to be further improved. Regarding the volume average particle size of inorganic fillers, the particle size distribution of the volume reference measured by a laser scattering diffraction particle size distribution measuring device can be determined as the particle size (D50) when the cumulative particle size distribution from the small diameter side reaches 50%.

[0128] From the viewpoint of improving filling performance in narrow gaps, such as when epoxy resin compositions are used for underfilling in molding, the maximum particle size (cut point) of the inorganic filler is preferably controlled. The maximum particle size of the inorganic filler can be appropriately adjusted; from the viewpoint of filling performance, it is preferably less than or equal to 105 μm, more preferably less than or equal to 75 μm, and may also be less than or equal to 60 μm, or even less than or equal to 40 μm. The maximum particle size can be measured using a laser diffraction particle size analyzer (manufactured by Horiba Manufacturing Co., Ltd., trade name: LA920).

[0129] (Specific silane compounds)

[0130] The epoxy resin composition according to the second embodiment contains a specific silane compound. The specific silane compound has a structure formed by combining a chain hydrocarbon group with 6 or more carbon atoms (hereinafter, a chain hydrocarbon group with 6 or more carbon atoms is also simply referred to as a chain hydrocarbon group) with silicon atoms. The chain hydrocarbon group may be branched or may have substituents. It should be noted that, in this disclosure, the number of carbon atoms in the chain hydrocarbon group refers to the number of carbon atoms without branches or substituents. The chain hydrocarbon group may or may not contain unsaturated bonds, but preferably does not contain unsaturated bonds.

[0131] It is believed that certain silane compounds function as coupling agents for inorganic fillers in epoxy resin compositions.

[0132] There are no particular restrictions on the atoms or groups of atoms bonded to the silicon atom, other than the chain hydrocarbon group. They can be hydrogen atoms, alkyl groups with 1 to 5 carbon atoms, alkoxy groups, aryl groups, aryloxy groups, etc. Preferably, in addition to the chain hydrocarbon group, one or more alkoxy groups are bonded to the silicon atom. More preferably, one chain hydrocarbon group and three alkoxy groups are bonded to the silicon atom.

[0133] The chain hydrocarbon group of a particular silane compound has 6 or more carbon atoms, and from the viewpoint of suppressing viscosity, it is preferable to have 7 or more carbon atoms, and more preferably 8 or more carbon atoms. There is no particular upper limit to the number of carbon atoms in the chain hydrocarbon group of a particular silane compound, but from the viewpoint of dispersibility in resin and the balance of physical properties of cured product, it is preferable to have 12 or more carbon atoms, more preferably 11 or more carbon atoms, and even more preferably 10 or more carbon atoms.

[0134] When a chain hydrocarbon group has substituents, the substituents are not particularly limited. Substituents can be present at the end of the chain hydrocarbon group or on the side chain of the chain hydrocarbon group.

[0135] The chain hydrocarbon group preferably has at least one functional group selected from (meth)acryloyl, epoxy, and alkoxy (hereinafter also referred to as a specific functional group), more preferably has at least one functional group selected from (meth)acryloyl and epoxy, and even more preferably has a (meth)acryloyl group. The specific functional group may be present at the end of the chain hydrocarbon group or in the side chain of the chain hydrocarbon group. From the viewpoint of suppressing viscosity, the specific functional group is preferably present at the end of the chain hydrocarbon group.

[0136] If the chain hydrocarbon groups in a particular silane compound possess specific functional groups, there is a tendency for the viscosity of the epoxy resin composition to decrease further. While the reason may not be clear, it is speculated that when the chain hydrocarbon groups in a particular silane compound possess specific functional groups, the compatibility of these functional groups with the epoxy resin increases, and the dispersibility of the epoxy resin with inorganic fillers improves.

[0137] When the chain hydrocarbon group has a (meth)acryloyl group, the (meth)acryloyl group can be directly bonded to the chain hydrocarbon group or bonded through other atoms or groups. For example, the chain hydrocarbon group can also have a (meth)acryloyloxy group. Preferably, the chain hydrocarbon group has a methacryloyloxy group.

[0138] When the chain hydrocarbon group has an epoxy group, the epoxy group can be directly bonded to the chain hydrocarbon group or bonded through other atoms or groups. For example, the chain hydrocarbon group can also have glycidyloxy groups, alicyclic epoxy groups, etc. Among them, the chain hydrocarbon group preferably has a glycidyloxy group.

[0139] When the chain hydrocarbon group has an alkoxy group, the alkoxy group can be directly bonded to the chain hydrocarbon group or bonded through other atoms or groups of atoms; it is preferred that it be directly bonded to the chain hydrocarbon group. The alkoxy group is not particularly limited and can be methoxy, ethoxy, propoxy, isopropoxy, etc. From the viewpoint of ease of acquisition, the chain hydrocarbon group preferably has a methoxy group.

[0140] There is no particular limitation on the equivalent (molecular weight / number of functional groups) of at least one functional group selected from (meth)acryloyl, epoxy, and alkoxy in a specific silane compound. From the viewpoint of reducing the viscosity of the epoxy resin composition, 200 g / eq to 420 g / eq is preferred, more preferably 210 g / eq to 405 g / eq, and even more preferably 230 g / eq to 390 g / eq.

[0141] Examples of specific silane compounds include: hexyltrimethoxysilane, heptyltrimethoxysilane, octyltrimethoxysilane, hexyltriethoxysilane, heptyltriethoxysilane, octyltriethoxysilane, 6-glycidoxyhexyltrimethoxysilane, 7-glycidoxyheptyltrimethoxysilane, 8-glycidoxyoctyltrimethoxysilane, 6-(meth)acryloyloxyhexyltrimethoxysilane, 7-(meth)acryloyloxyheptyltrimethoxysilane, 8-(meth)acryloyloxyoctyltrimethoxysilane, and decyltrimethoxysilane. Among these, 8-glycidoxyoctyltrimethoxysilane and 8-methacryloyloxyoctyltrimethoxysilane are preferred from the viewpoint of reducing the viscosity of the epoxy resin composition. A single specific silane compound may be used, or two or more may be used in combination.

[0142] Certain silane compounds can be synthesized or commercially available silane compounds can be used. Examples of commercially available silane compounds include KBM-3063 (hexyltrimethoxysilane), KBE-3063 (hexyltriethoxysilane), KBE-3083 (octyltriethoxysilane), KBM-4803 (8-glycidoxyoctyltrimethoxysilane), KBM-5803 (8-methacryloyloxyoctyltrimethoxysilane), and KBM-3103C (decyltrimethoxysilane), all manufactured by Shin-Etsu Chemical Co., Ltd.

[0143] The content of the specific silane compound in the epoxy resin composition according to the second embodiment is not particularly limited. The content of the specific silane compound relative to 100 parts by weight of the inorganic filler can be greater than or equal to 0.01 parts by weight, or greater than or equal to 0.02 parts by weight. Furthermore, the content of the specific silane compound relative to 100 parts by weight of the inorganic filler is preferably less than or equal to 5 parts by weight, more preferably less than or equal to 2.5 parts by weight. If the content of the specific silane compound relative to 100 parts by weight of the inorganic filler is greater than or equal to 0.01 parts by weight, there is a tendency to obtain a composition with low viscosity. If the content of the specific silane compound relative to 100 parts by weight of the inorganic filler is less than or equal to 5 parts by weight, there is a tendency to further improve the moldability of the encapsulation.

[0144] (Other coupling agents)

[0145] The epoxy resin composition according to the second embodiment may further contain other coupling agents in addition to the specific silane compound. There are no particular limitations on the other coupling agents, as long as they are coupling agents commonly used in epoxy resin compositions. Examples of other coupling agents include silane compounds (excluding the specific silane compound) such as epoxy silanes, mercaptosilanes, aminosilanes, alkylsilanes, ureosilanes, and vinylsilanes, as well as titanium compounds, aluminum chelate compounds, and aluminum / zirconium compounds. Other coupling agents may be used alone or in combination of two or more.

[0146] When the epoxy resin composition according to the second embodiment contains coupling agents other than a specific silane compound, the total content of the specific silane compound and other coupling agents relative to 100 parts by weight of the inorganic filler can be greater than or equal to 0.01 parts by weight, or greater than or equal to 0.02 parts by weight. Furthermore, the total content of the specific silane compound and other coupling agents relative to 100 parts by weight of the inorganic filler is preferably less than or equal to 5 parts by weight, more preferably less than or equal to 2.5 parts by weight. If the total content of the specific silane compound and other coupling agents relative to 100 parts by weight of the inorganic filler is greater than or equal to 0.01 parts by weight, there is a tendency to obtain a composition with low viscosity. If the total content of the specific silane compound and other coupling agents relative to 100 parts by weight of the inorganic filler is less than or equal to 5 parts by weight, there is a tendency to further improve the moldability of the encapsulation.

[0147] In the case where the epoxy resin composition according to the second embodiment contains coupling agents other than a specific silane compound, from the viewpoint of effectively utilizing the specific silane compound, the content of the other coupling agents is preferably less than or equal to 90% by mass, more preferably less than or equal to 70% by mass, and even more preferably less than or equal to 50% by mass relative to the total amount of the specific silane compound and the other coupling agents.

[0148] (Curing accelerator)

[0149] The epoxy resin composition according to the second embodiment may also contain a curing accelerator. Details of the curing accelerator are the same as those of the curing accelerator used in the epoxy resin composition according to the first embodiment.

[0150] [Various additives]

[0151] In addition to the components described above, the epoxy resin composition according to the second embodiment may also contain various additives such as ion exchangers, mold release agents, flame retardants, colorants, and stress relievers. Details of these additives are the same as those for the additives used in the epoxy resin composition according to the first embodiment.

[0152] [Physical Properties of Epoxy Resin Compositions]

[0153] The physical properties of the epoxy resin compositions according to the first and second embodiments of this disclosure will be described below.

[0154] (Viscosity of the epoxy resin composition)

[0155] There are no particular limitations on the viscosity of the epoxy resin composition. However, the ease with which lead wire deflection occurs during molding varies depending on the molding method and the composition of the epoxy resin composition. Therefore, it is preferable to adjust the viscosity according to the molding method and the composition of the epoxy resin composition to achieve the desired viscosity.

[0156] For example, when molding the epoxy resin composition by compression molding, from the viewpoint of reducing lead wire offset, it is preferable that the viscosity at 175°C be less than or equal to 200 Pa·s, more preferably less than or equal to 150 Pa·s, even more preferably less than or equal to 100 Pa·s, particularly preferably less than or equal to 50 Pa·s, and may also be less than or equal to 16 Pa·s, or even less than or equal to 10 Pa·s. The lower limit of viscosity is not particularly limited; for example, it may be greater than or equal to 5 Pa·s.

[0157] Furthermore, when molding the epoxy resin composition by transfer molding, for example, from the viewpoint of reducing lead wire offset, it is preferable that the viscosity at 175°C be less than or equal to 200 Pa·s, more preferably less than or equal to 150 Pa·s, even more preferably less than or equal to 100 Pa·s, and may also be less than or equal to 68 Pa·s, or may also be less than or equal to 54 Pa·s. The lower limit of viscosity is not particularly limited, for example, it may be greater than or equal to 5 Pa·s.

[0158] The viscosity of the epoxy resin composition can be measured using a high-performance flow tester (manufactured by Shimadzu Corporation).

[0159] (Thermal conductivity when the product is cured)

[0160] There are no particular limitations on the thermal conductivity when the epoxy resin composition is cured. From the viewpoint of obtaining the desired heat dissipation, it can be greater than or equal to 3.0 W / (m·K), 4.0 W / (m·K), 5.0 W / (m·K), 6.0 W / (m·K), 7.0 W / (m·K), or 8.0 W / (m·K) at room temperature (25°C). There is no particular upper limit to the thermal conductivity, and it can be 9.0 W / (m·K).

[0161] The thermal conductivity of the cured material can be measured by the xenon flash method (manufactured by NETZSCH, trade name LFA467 Hyper Flash device).

[0162] [Method for preparing epoxy resin composition]

[0163] The preparation methods of the epoxy resin compositions according to the first and second embodiments are not particularly limited. As a general method, examples include thoroughly mixing the components using a mixer or the like, then melt-kneading using a grinding roller, extruder, or the like, followed by cooling and pulverizing. More specifically, examples include stirring and mixing the aforementioned components, then kneading, cooling, and pulverizing using a kneader, roller, extruder, or the like preheated to 70°C to 140°C.

[0164] The epoxy resin composition can be in a solid or liquid state at room temperature and pressure (e.g., 25°C, atmospheric pressure), but is preferably solid. When the epoxy resin composition is solid, there are no particular limitations on its shape; examples include powder, granules, and tablets. From an operability point of view, the size and weight of the epoxy resin composition when it is in tablet form are preferably those that conform to the molding conditions for encapsulation.

[0165] <Electronic Components and Devices>

[0166] As one aspect of this disclosure, an electronic component device includes an element that has been sealed by the epoxy resin composition described in the first and second embodiments above.

[0167] As an electronic component device, an example is an electronic component device that is formed by sealing the component portion (active components such as semiconductor chips, transistors, diodes, thyristors, capacitors, resistors, coils, etc.) on a supporting component such as a lead frame, a wired carrier, a wiring board, glass, a silicon wafer, or an organic substrate using an epoxy resin composition.

[0168] More specifically, examples include: DIP (Dual Inline Package), PLCC (Plastic Leaded Chip Carrier), QFP (Quad Flat Package), SOP (Small Outline Package), SOJ (Small Outline J-lead package), TSOP (Thin Small Outline Package), and TQFP (Thin Quad Flat Package), etc., which are general resin-sealed ICs. These structures involve fixing components on a lead frame, connecting the terminals of components such as pads to the lead portions using wire bonding, bumps, etc., and then sealing them with an epoxy resin composition through transfer molding, etc.; TCP (Tape Carrier Package), which has a structure that seals components connected to the carrier using bumps with an epoxy resin composition; and COB (Chip On Board), which has the following structures. Board (on-board chip) modules, hybrid ICs, multi-chip modules, etc., are structures formed by sealing components connected to wiring formed on a support member via wire bonding, flip chip bonding, solder, etc., using an epoxy resin composition. BGA (Ball Grid Array), CSP (Chip Size Package), MCP (Multi Chip Package), etc., have structures where components are mounted on the surface of a support member with wiring board connection terminals formed on the back side. The components are connected to wiring formed on the support member via bumps or wire bonding, and then the components are sealed using an epoxy resin composition. Epoxy resin compositions can also be suitably used in printed circuit boards.

[0169] Methods for sealing electronic components using epoxy resin compositions include low-pressure transfer molding, injection molding, and compression molding.

[0170] Example

[0171] The above embodiments will be specifically described below through examples, but the scope of the above embodiments is not limited to these examples.

[0172] Embodiments relating to the first implementation

[0173] <Preparation of Resin Composition>

[0174] First, prepare the ingredients shown below.

[0175] [Epoxy Resin 1 (E1)] Manufactured by Mitsubishi Chemical Corporation, JER YX-4000H (trade name)

[0176] [Epoxy Resin 2 (E2)] Nippon Steel & Sumitomo Chemical Co., Ltd. EPOTOHTO YSLV-80XY (Trade Name)

[0177] [Epoxy Resin 3 (E3)] Nippon Steel & Sumitomo Chemical Co., Ltd. EPOTOHTO YSLV-70XY (Trade Name)

[0178] [Curing Agent 1 (H1)] H-4 (trade name) manufactured by Meiwa Kasei Corporation

[0179] [Curing Agent 2 (H2)] Nippon Steel & Sumitomo Chemical Co., Ltd. SN-485 (trade name)

[0180] [Curing Agent 3 (H3)] MEH-7851SS manufactured by Meiwa Kasei Corporation (trade name)

[0181] [Cure Accelerator 1 (C1)] adduct of tri-p-tolylphosphine and 1,4-benzoquinone

[0182] [Cure Accelerator 2 (C2)] Triphenylphosphine and 1,4-benzoquinone adduct

[0183] [Inorganic filler 1 (A1)] Ultrafine alumina with an average particle size of 0.2 μm

[0184] [Inorganic filler 2 (A2)] Fine alumina with an average particle size of 1 μm and a cut point of 25 μm.

[0185] [Inorganic filler 3 (A3)] Alumina with a median diameter of 20 μm and a cleavage point of 35 μm.

[0186] [Inorganic filler 4 (A4)] Alumina with a median diameter of 13 μm and a cleavage point of 55 μm.

[0187] [Inorganic filler 5 (A5)] Alumina with an average particle size of 11 μm and a cut point of 75 μm.

[0188] [Inorganic filler 6 (A6)] Silica with an average particle size of 3 μm and a cut point of 10 μm.

[0189] [Inorganic filler 7 (A7)] Silicon dioxide with a median diameter of 4 μm and a cut point of 20 μm

[0190] [Silane Compound 1] N-Phenylon-3-aminopropyltrimethoxysilane; KBM-573 (trade name, manufactured by Shin-Etsu Chemical Co., Ltd.)

[0191] [Silane Compound 2] Methyltrimethoxysilane; KBM-13 (trade name, manufactured by Shin-Etsu Chemical Co., Ltd.)

[0192] [Silane Compound 3] n-Propyltrimethoxysilane; KBM-3033 (trade name, manufactured by Shin-Etsu Chemical Co., Ltd.)

[0193] [Silane Compound 4] Hexyltrimethoxysilane; KBM-3063 (trade name, manufactured by Shin-Etsu Chemical Co., Ltd.)

[0194] [Silane Compound 5] Octyltriethoxysilane; KBE-3083 (trade name, manufactured by Shin-Etsu Chemical Co., Ltd.)

[0195] [Silane Compound 6] 8-Glycidoxyoctyltrimethoxysilane; KBM-4803 (trade name, manufactured by Shin-Etsu Chemical Co., Ltd.)

[0196] [Silane Compound 7] 8-Methacryloyloxyoctyltrimethoxysilane; KBM-5803 (trade name, manufactured by Shin-Etsu Chemical Co., Ltd.)

[0197] [Silane Compound 8] Decyltrimethoxysilane; KBM-3103C (trade name, manufactured by Shin-Etsu Chemical Co., Ltd.)

[0198] The components shown in Tables 1 and 2 were combined in the amounts shown in the tables (parts by mass) and thoroughly mixed using a mixer. The mixture was then melt-mixed at 100°C for 2 minutes using a twin-screw extruder. Next, the melt was cooled, and the solidified material was pulverized into a powder to prepare the target powdered epoxy resin composition. In the tables, blank columns indicate that no components were combined, and "-" indicates that no evaluation was performed.

[0199] The prepared epoxy resin compositions were evaluated through various tests shown below. The evaluation results are shown in Tables 1 and 2. It should be noted that the epoxy resin compositions described in Examples A-1 to A-7 and Comparative Examples A-1 to A-3 were molded using a compression molding machine, while the epoxy resin compositions described in Examples A-8 to A-17 and Comparative Examples A-4 to A-5 were molded using a transfer molding machine.

[0200] <Viscosity Evaluation>

[0201] The lowest melt viscosity at 175°C was determined using the epoxy resin compositions described in Examples A-1 to A-17 and Comparative Examples A-1 to A-5. The results are shown in Tables 1 and 2 below. The lowest melt viscosity was determined using a high-performance flow tester (manufactured by Shimadzu Corporation).

[0202] <Evaluation of lead offset>

[0203] Using the epoxy resin compositions described in Examples A-1 to A-7 and Comparative Examples A-1 to A-3, the package was sealed using a compression molding machine (TOWA, PMC-1040S) at a molding temperature of 175°C and a molding time of 120 seconds, followed by post-curing at 175°C for 5 hours to obtain a semiconductor device. This semiconductor device is a ball grid array (BGA) package (resin-sealed portion dimensions: 228mm × 67mm × thickness 1mm), with a chip size of 7.5mm × 7.5mm. Regarding the leads, the gold wire diameter is 18μm, and the average gold wire length is 5mm. The deformability of the gold wire leads was then observed using a soft X-ray diffraction apparatus to check for any deformation.

[0204] Furthermore, using the epoxy resin compositions described in Examples A-8 to A-17 and Comparative Examples A-4 to A-5, the package was sealed using a transfer molding machine (Manual-Press Y-1, TOWA Corporation) at a molding temperature of 175°C and a molding time of 120 seconds, followed by post-curing at 175°C for 5 hours to obtain a semiconductor device. This semiconductor device is a ball grid array (BGA) package (resin-sealed portion dimensions: 50mm × 50mm × thickness 0.7mm), with a chip size of 7.5mm × 7.5mm. Regarding the leads, the gold wire diameter is 22μm, and the average gold wire length is 3mm. Then, the deformation state of the gold wire leads was observed using a soft X-ray analysis device to check for any deformation.

[0205] The evaluation will be conducted according to the following criteria.

[0206] AA: The occurrence rate of lead wire misalignment is less than 3%.

[0207] A: The occurrence rate of lead wire misalignment is greater than or equal to 3% and less than 5%.

[0208] B: The occurrence rate of lead wire misalignment is greater than or equal to 5% and less than 7%.

[0209] C: The occurrence rate of lead wire misalignment is greater than or equal to 7%.

[0210] <Evaluation of the filling performance of molded underfill (MUF)>

[0211] Using the epoxy resin compositions described in Examples A-1 to A-7 and Comparative Examples A-1 to A-3, a semiconductor device was formed using a compression molding machine (TOWA, PMC-1040S) at a molding temperature of 175°C, a die gap of 2 mm, a vacuum holding time of 6 seconds, and a molding time of 120 seconds. The infill performance of the flip chip was evaluated. The semiconductor device was a ball grid array (BGA) package (resin seal dimensions: 228 mm × 67 mm × 1 mm thickness), and the chip size was 7.5 mm × 7.5 mm. The flip chip bump size was 60 μm, calculated by combining 45 μm Cu pillars and 15 μm solder bumps. To evaluate infill performance, an ultrasonic testing device was used to check for any voids in the under-chip gap.

[0212] Let A be the case with good filling performance, and let C be the case with unfilled parts such as pores.

[0213] <Evaluation of thermal conductivity>

[0214] The epoxy resin compositions described in Examples A-1 to A-17 and Comparative Examples A-1 to A-5 were molded using a high-temperature vacuum molding machine at 175°C, 600 seconds, and 7 MPa. The test pieces with a thickness of 1 mm and a square of 10 mm were measured at room temperature using a NETZSCH LFA467 HyperFlash device. The value calculated by the xenon flash method was set as the thermal conductivity.

[0215] [Table 1]

[0216]

[0217] [Table 2]

[0218]

[0219] According to the results in Tables 1 and 2, the epoxy resin compositions of the examples containing silane compounds with a structure formed by the combination of chain hydrocarbon groups with 6 or more carbon atoms and silicon atoms exhibit lower viscosity and a lower incidence of lead wire deflection compared to the comparative examples. Furthermore, the epoxy resin compositions of the examples containing silane compounds with a structure formed by the combination of chain hydrocarbon groups with 6 or more carbon atoms and silicon atoms show excellent filling properties when used as underfill in molding by compression molding. In particular, when the number of carbon atoms in the chain hydrocarbon groups is greater than or equal to 8, there is a tendency for excellent thermal conductivity when the cured product is formed.

[0220] Embodiments relating to the second implementation

[0221] <Preparation of Resin Composition>

[0222] First, prepare the components shown below. It should be noted that the thermal conductivity of inorganic fillers 1 through 3 is all greater than or equal to 20 W / (m·K).

[0223] [Epoxy Resin 1 (E1)] Manufactured by Mitsubishi Chemical Corporation, jER YX-4000H (trade name)

[0224] [Epoxy Resin 2 (E2)] Manufactured by Nippon Steel & Sumitomo Chemical Co., Ltd., EPOTOHTO YSLV-80XY (trade name)

[0225] [Curing Agent 1 (H1)] Manufactured by Meiwa Kasei Corporation, H-4 (trade name)

[0226] [Curing Agent 2 (H2)] Nippon Steel & Sumitomo Chemical Co., Ltd. SN-485 (trade name)

[0227] [Cure Accelerator 1 (C1)] adduct of tri-p-tolylphosphine and 1,4-benzoquinone

[0228] [Inorganic filler 1 (A1)] Ultrafine alumina with an average particle size of 0.2 μm

[0229] [Inorganic filler 2 (A2)] Alumina with a median diameter of 13 μm and a cleavage point of 55 μm.

[0230] [Inorganic filler 3 (A3)] Alumina with an average particle size of 11 μm and a cut point of 75 μm.

[0231] [Silane Compound 1] N-Phenylon-3-aminopropyltrimethoxysilane; KBM-573 (trade name, manufactured by Shin-Etsu Chemical Co., Ltd.)

[0232] [Silane Compound 2] Hexyltrimethoxysilane; KBM-3063 (trade name, manufactured by Shin-Etsu Chemical Co., Ltd.)

[0233] [Silane Compound 3] Octyltriethoxysilane; KBE-3083 (trade name, manufactured by Shin-Etsu Chemical Co., Ltd.)

[0234] [Silane Compound 4] 8-Glycidoxyoctyltrimethoxysilane; KBM-4803 (trade name, manufactured by Shin-Etsu Chemical Co., Ltd.)

[0235] [Silane Compound 5] 8-Methacryloyloxyoctyltrimethoxysilane; KBM-5803 (trade name, manufactured by Shin-Etsu Chemical Co., Ltd.)

[0236] [Silane Compound 6] Decyltrimethoxysilane; KBM-3103C (trade name, manufactured by Shin-Etsu Chemical Co., Ltd.)

[0237] The components shown in Tables 3 and 4 were combined in the amounts shown in the tables (parts by mass) and thoroughly mixed using a mixer. The mixture was then melt-blended at 100°C for 2 minutes using a twin-screw extruder. Next, the melt was cooled and then pulverized into a powder to prepare the target powdered epoxy resin composition. In the tables, blank columns indicate that no components were combined, and "-" indicates that no evaluation was performed.

[0238] The prepared epoxy resin compositions were evaluated through various tests shown below. The evaluation results are shown in Tables 3 and 4. It should be noted that the molding of Examples B-1 to B-10 and Comparative Examples B-1 to B-2 was performed using a transfer molding machine.

[0239] <Viscosity Evaluation>

[0240] The lowest melt viscosity at 175°C was determined using the epoxy resin compositions of the Examples and Comparative Examples. The results are shown in Tables 3 and 4 below. The lowest melt viscosity was determined using a high-performance flow tester (manufactured by Shimadzu Corporation).

[0241] <Evaluation of lead offset>

[0242] Using the epoxy resin compositions of the examples and comparative examples, the package was sealed using a transfer molding machine (TOWA, Manual-Press Y-1) at a molding temperature of 175°C and a molding time of 120 seconds, followed by post-curing at 175°C for 5 hours to obtain a semiconductor device. This semiconductor device is a ball grid array (BGA) package (resin-sealed portion dimensions: 50mm × 50mm × thickness 0.7mm), with a chip size of 7.5mm × 7.5mm. Regarding the leads, the gold wire diameter is 22μm, and the average gold wire length is 3mm. The fabricated package was then inspected for deformation of the gold wire leads using a soft X-ray diffraction apparatus to check for any deformation.

[0243] The evaluation will be conducted according to the following criteria.

[0244] AA: The occurrence rate of lead wire misalignment is less than 3%.

[0245] A: The occurrence rate of lead wire misalignment is greater than or equal to 3% and less than 5%.

[0246] B: The occurrence rate of lead wire misalignment is greater than or equal to 5% and less than 7%.

[0247] C: The occurrence rate of lead wire misalignment is greater than or equal to 7%.

[0248] <Evaluation of thermal conductivity>

[0249] The epoxy resin compositions of the examples and comparative examples were molded using a high-temperature vacuum molding machine at 175°C, 600 seconds, and 7 MPa. The test pieces with a thickness of 1 mm and a square of 10 mm were measured at room temperature using a NETZSCH LFA467 Hyper Flash device. The value calculated by the xenon flash method was set as the thermal conductivity.

[0250] [Table 3]

[0251]

[0252] [Table 4]

[0253]

[0254] As can be seen from the results of the examples, the epoxy resin compositions of the examples containing alumina and silane compounds having a structure in which chain hydrocarbon groups with a carbon number greater than or equal to 6 carbon atoms are bonded to silicon atoms have low viscosity and excellent thermal conductivity when the cured product is formed. In particular, when the chain hydrocarbon groups have a carbon number greater than or equal to 8 carbon atoms, the thermal conductivity when the cured product is formed is improved.

[0255] The disclosures of Japanese Patent Application No. 2017-178299 and Japanese Patent Application No. 2017-178300 are incorporated herein by reference in their entirety.

[0256] All documents, patent applications and technical standards described in this specification are incorporated herein by reference to the same extent as the specific documents, patent applications and technical standards which are incorporated herein by reference.

Claims

1. An epoxy resin composition, used as a compression molding sealant or a transfer molding sealant, comprising an epoxy resin, a curing agent, an inorganic filler, and a silane compound, wherein the silane compound has a structure formed by the bonding of chain hydrocarbon groups with 6 or more carbon atoms to silicon atoms, and the epoxy resin composition is a solid in powder, granule, or tablet form at 25°C and atmospheric pressure. The silane compound is selected from at least one group consisting of hexyltrimethoxysilane, heptyltrimethoxysilane, octyltrimethoxysilane, hexyltriethoxysilane, heptyltriethoxysilane, octyltriethoxysilane, and decyltrimethoxysilane.

2. The epoxy resin composition according to claim 1, wherein the content of the inorganic filler in the epoxy resin composition is 30% to 99% by volume.

3. The epoxy resin composition according to claim 1, wherein the thermal conductivity of the inorganic filler is greater than or equal to 20 W / (m·K).

4. The epoxy resin composition according to claim 3, wherein the inorganic filler having a thermal conductivity greater than or equal to 20 W / (m·K) comprises at least one selected from the group consisting of alumina, silicon nitride, boron nitride, aluminum nitride, magnesium oxide, and silicon carbide.

5. The epoxy resin composition according to claim 1, wherein the inorganic filler content in the epoxy resin composition is greater than or equal to 50% by volume.

6. An electronic component device comprising an element sealed with the epoxy resin composition according to any one of claims 1 to 5.

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