Epoxy resin composition for sealing, electronic component device, and method for manufacturing the same.

Abstract

An epoxy resin composition for sealing, according to the present invention, contains an epoxy resin, a phenol curing agent, an inorganic filler, and triazine ring-containing compound, and the content of the phenol curing agent is 40 wt. % to 250 wt. % relative to 100 wt. % of the epoxy resin, or the total content of the epoxy resin and the phenol curing agent relative to the total content of tetrahydrofuran soluble solids in the epoxy resin compound is 85 wt. % or more, the epoxy resin compound further containing a hydrotalcite compound in one aspect.

Description

[Technical Field]

[0001] This disclosure relates to an epoxy resin composition for sealing, an electronic component device, and a method for manufacturing the same. [Background technology]

[0002] Various semiconductor elements used in electronic components such as transistors and ICs (Integrated Circuits) are predominantly sealed with resin due to factors such as productivity and manufacturing cost. Epoxy resin compositions are widely used as sealing materials. This is because epoxy resins offer an excellent balance of various properties required for sealing materials, including workability, moldability, electrical properties, moisture resistance, heat resistance, mechanical properties, and adhesion to inserts.

[0003] Patent Document 1 describes a semiconductor encapsulation resin composition containing an epoxy resin, a benzoxazine resin, a phenol curing agent, a curing accelerator, an inorganic filler, and a specific silicon-containing triazine compound in an amount of 0.05% to 2% by mass relative to the total amount of the composition. The resin composition described in Patent Document 1 improves reflow resistance, heat resistance, and moldability, as well as adhesion to insert parts, by curing the epoxy resin with the benzoxazine resin and the phenol curing agent.

[0004] Furthermore, epoxy resin compositions typically contain ionic impurities such as organic acid ions and chloride ions derived from the raw materials of the epoxy resin. These ionic impurities can cause corrosion of metal components such as wires, leading to a decrease in the moisture resistance reliability of electronic components. Therefore, to improve the moisture resistance reliability of electronic components, ion exchangers such as hydrotalcite compounds are sometimes included in the epoxy resin composition for sealing (see, for example, Patent Documents 1 and 2). [Prior art documents] [Patent Documents]

[0005] [Patent Document 1] Japanese Patent Publication No. 2019-172911 [Patent Document 2] Japanese Patent Publication No. 2015-44898 [Overview of the Initiative] [Problems that the invention aims to solve]

[0006] Epoxy resin compositions used for sealing lose their curability when they absorb moisture from the air; therefore, material designs are generally created to minimize moisture absorption. For example, if a high content of silane coupling agent is added to an epoxy resin composition to improve adhesion to components, the amount of water absorbed may increase, leading to a decrease in curability. Similarly, adding a high content of alumina filler for purposes such as high thermal conductivity may also reduce moisture-absorbing curability. Consequently, the degree of freedom in designing the composition of epoxy resin compositions has sometimes been limited from the standpoint of moisture-absorbing curability. Furthermore, epoxy resin compositions used for sealing are generally hermetically sealed and used within a certain period after opening to prevent deterioration due to moisture absorption. On the other hand, it is desirable to reduce these limitations, increase the degree of freedom in designing various components, and broaden the tolerance range for management.

[0007] In view of the above circumstances, the first and second embodiments of this disclosure aim to provide an epoxy resin composition for sealing that exhibits excellent moisture-absorbing and curing properties, as well as an electronic component device comprising a cured product of the epoxy resin composition for sealing and a method for manufacturing the same.

[0008] Furthermore, it is desirable to reduce the content of ionic impurities in the epoxy resin composition and further improve the moisture resistance reliability of electronic component devices.

[0009] Patent Document 1 describes a semiconductor encapsulation resin composition containing an epoxy resin, a benzoxazine resin, a phenol curing agent, a curing accelerator, an inorganic filler, and a specific silicon-containing triazine compound. Patent Document 1 also states that stabilizers such as hydrotalcite may be added to the resin composition. However, Patent Document 1 does not focus on improving moisture resistance reliability by reducing the amount of ionic impurities.

[0010] Furthermore, Patent Document 2 describes an epoxy resin composition for semiconductor encapsulation that incorporates an uncalcined hydrotalcite-like compound for the purpose of improving reliability. However, further improvements are desired in the moisture resistance reliability of electronic component devices.

[0011] In view of the above circumstances, the third and fourth embodiments of this disclosure aim to provide an epoxy resin composition for sealing that can produce an electronic component device with high moisture resistance, as well as an electronic component device comprising a cured product of the epoxy resin composition and a method for manufacturing the same. [Means for solving the problem]

[0012] The means for solving the above problems include the following embodiments. <1> It contains epoxy resin, a phenol curing agent, an inorganic filler, and a triazine ring-containing compound. The content of the phenol curing agent is 40 to 250 parts by mass per 100 parts by mass of the epoxy resin. Epoxy resin composition for sealing. <2> It contains epoxy resin, a phenol curing agent, an inorganic filler, and a triazine ring-containing compound. The total mass of the epoxy resin and the phenol curing agent is 85% by mass or more, relative to the total mass of tetrahydrofuran-soluble solids in the epoxy resin composition for sealing. Epoxy resin composition for sealing. <3> It contains epoxy resin, phenol curing agent, inorganic filler, triazine ring-containing compound, and hydrotalcite compound. The content of the phenol curing agent is 40 to 250 parts by mass per 100 parts by mass of the epoxy resin. Epoxy resin composition for sealing. <4> It contains epoxy resin, phenol curing agent, inorganic filler, triazine ring-containing compound, and hydrotalcite compound. The total mass of the epoxy resin and the phenol curing agent is 85% by mass or more, relative to the total mass of tetrahydrofuran-soluble solids in the epoxy resin composition for sealing. Epoxy resin composition for sealing. <5> The ratio of the number of hydroxyl groups in the phenol curing agent to the number of epoxy groups in the epoxy resin in the encapsulating epoxy resin composition (number of hydroxyl groups in the phenol curing agent / number of epoxy groups in the epoxy resin) is 0.8 to 1.2. <1> ~ <4> An epoxy resin composition for sealing according to any one of the items. <6> The epoxy resin comprises at least one selected from the group consisting of aralkyl epoxy resins and biphenyl epoxy resins. <1> ~ <5> An epoxy resin composition for sealing according to any one of the items. <7> The triazine ring of the triazine ring-containing compound has a substituent, and the substituent includes a primary amino group. <1> ~ <6> An epoxy resin composition for sealing according to any one of the items. <8> The triazine ring-containing compound includes a compound represented by the following formula (I), where Y represents a monovalent organic group having 1 to 30 carbon atoms and a hydroxyl group, or a monovalent organic group having 1 to 30 carbon atoms and an alkoxysilyl group. <1> ~ <7> An epoxy resin composition for sealing according to any one of the items.

[0013] [ka]

[0014] <9> The content of the triazine ring-containing compound is 0.3 parts by mass to 20 parts by mass per 100 parts by mass of the epoxy resin. <1> ~ <8> An epoxy resin composition for sealing according to any one of the items. <10> Furthermore, it contains 2.0% by mass or more of a silane coupling agent relative to the total mass of the epoxy resin and the phenol curing agent. <1> ~ <9> An epoxy resin composition for sealing according to any one of the items. <11> Element and, The aforementioned button is sealed. <1> ~ <10> A cured product of the encapsulating epoxy resin composition described in any one of the items, An electronic component device equipped with the following features. <12> <1> ~ <10> A method for manufacturing an electronic component device, comprising sealing an element with an epoxy resin composition for sealing as described in any one of the items. [Effects of the Invention]

[0015] According to the first and second embodiments of this disclosure, an epoxy resin composition for sealing that exhibits excellent moisture-absorbing and curing properties, and an electronic component device comprising a cured product of the epoxy resin composition for sealing, and a method for manufacturing the same are provided.

[0016] According to the third and fourth embodiments of this disclosure, there are provided an epoxy resin composition for sealing that can produce an electronic component device with high moisture resistance, as well as an electronic component device comprising a cured product of the epoxy resin composition and a method for manufacturing the same. [Modes for carrying out the invention]

[0017] The embodiments for carrying out the present invention will be described in detail below. However, the embodiments of this disclosure are not limited to the following embodiments. In the following embodiments, the components (including elemental steps, etc.) are not essential unless otherwise specified. The same applies to numerical values ​​and their ranges, and do not limit the embodiments of this disclosure.

[0018] In this disclosure, the term "process" includes not only processes that are independent of other processes, but also processes that cannot be clearly distinguished from other processes, provided that the purpose of such process is achieved. In this disclosure, the numerical range indicated using "~" includes the numbers before and after "~" as the minimum and maximum values, respectively. In numerical ranges described in stages within this disclosure, the upper or lower limit of one numerical range may be replaced with the upper or lower limit of another numerical range described in stages. Furthermore, in numerical ranges described within this disclosure, the upper or lower limit of that range may be replaced with the values ​​shown in the examples. In this disclosure, each component may contain multiple types of the corresponding substance. If multiple types of the substance corresponding to each component are present in the composition, the content or amount of each component means the total content or amount of the multiple types of substances present in the composition, unless otherwise specified. In this disclosure, each component may contain multiple types of particles. If multiple types of particles corresponding to each component are present in the composition, the particle size of each component refers to the value for a mixture of such multiple types of particles present in the composition, unless otherwise specified.

[0019] In this disclosure, unless otherwise specified, the number of carbon atoms in an organic group refers to the number of carbon atoms including those of substituents if the organic group includes substituents.

[0020] <Epoxy resin compositions for sealing according to the first and second embodiments> An epoxy resin composition for sealing according to the first embodiment of this disclosure (hereinafter, the epoxy resin composition for sealing is also simply referred to as the epoxy resin composition) contains an epoxy resin, a phenol curing agent, an inorganic filler, and a triazine ring-containing compound, wherein the content of the phenol curing agent is 40 to 250 parts by mass per 100 parts by mass of the epoxy resin.

[0021] The epoxy resin composition for sealing according to the second embodiment of this disclosure contains an epoxy resin, a phenol curing agent, an inorganic filler, and a triazine ring-containing compound, wherein the total mass of the epoxy resin and the phenol curing agent is 85% by mass or more with respect to the total mass of tetrahydrofuran-soluble solids in the epoxy resin composition for sealing.

[0022] Through the inventors' investigations, it was found that the epoxy resin compositions according to the first and second embodiments exhibit excellent moisture-absorbing curability. Although the reason for this is not clear, it is presumed that in the reaction between the epoxy resin and the phenol curing agent according to the first and second embodiments, the triazine ring-containing compound contributes to the reaction to some extent, thereby suppressing the decrease in curability due to moisture absorption in the epoxy resin composition.

[0023] Furthermore, in one embodiment, it has been found that the epoxy resin compositions according to the first and second embodiments tend to exhibit excellent adhesion to metals such as copper and silver, in addition to their moisture-curing properties. It is thought that the nitrogen atom in the triazine ring of the triazine ring-containing compound contributes to the adhesion to metals. Generally, increasing the amount of silane coupling agent to improve adhesion tends to increase water absorption, and it tends to be difficult to achieve both adhesion and moisture-curing properties. Therefore, being able to achieve both excellent moisture-curing properties and adhesion is useful.

[0024] In addition, in one embodiment, it has been found that the epoxy resin compositions according to the first and second embodiments tend to have low electrical conductivity in their extracts. Normally, epoxy resin compositions contain ionic impurities such as organic acid ions and chloride ions, and these ionic impurities increase the electrical conductivity of the epoxy resin composition, which reduces the moisture resistance reliability of electronic components. On the other hand, it has been found that in the epoxy resin compositions according to the first and second embodiments, the amount of such ionic impurities in the extract is suppressed, and low electrical conductivity is maintained. As a result, it is expected that it will be possible to manufacture electronic components with high moisture resistance reliability.

[0025] The epoxy resin compositions according to the first and second embodiments may further contain additives and the like. The components that may be included in the epoxy resin compositions according to the first and second embodiments will be described in detail below.

[0026] <Epoxy resin> The epoxy resin composition contains an epoxy resin. The type of epoxy resin is not particularly limited as long as it has two or more epoxy groups in one molecule. The epoxy resin may be solid or liquid at 25°C and atmospheric pressure, but it is preferably solid. Specifically, these include: novolac-type epoxy resins (phenol novolac-type epoxy resins, orthocresol novolac-type epoxy resins, etc.) obtained by condensing or co-condensing a novolac resin obtained by condensing or co-condensing a novolac resin obtained by phenol compounds selected from the group consisting of phenol compounds such as phenol, cresol, xylenol, resorcinol, catechol, bisphenol A, bisphenol F, and naphthol compounds such as α-naphthol, β-naphthol, and dihydroxynaphthalene under an acidic catalyst; triphenylmethane-type epoxy resins obtained by condensing or co-condensing a triphenylmethane-type phenol resin obtained by condensing or co-condensing the above phenol compound with an aromatic aldehyde compound such as benzaldehyde and salicylaldehyde under an acidic catalyst; and novolac resins obtained by co-condensing the above phenol compound and naphthol compound with an aldehyde compound under an acidic catalyst. Copolymer epoxy resins; diphenylmethane type epoxy resins which are diglycidyl ethers of bisphenol A, bisphenol F, etc.; biphenyl type epoxy resins which are diglycidyl ethers of alkyl-substituted or unsubstituted biphenols; stilbene type epoxy resins which are diglycidyl ethers of stilbene-based phenol compounds; sulfur atom-containing epoxy resins which are diglycidyl ethers of bisphenol S, etc.; glycidyl ether type epoxy resins which are glycidyl ethers of alcohols such as butanediol, polyethylene glycol, and polypropylene glycol; glycidyl ester type epoxy resins which are glycidyl esters of polycarboxylic acid compounds such as phthalic acid, isophthalic acid, and tetrahydrophthalic acid; glycidylamine type epoxy resins in which the active hydrogen bonded to the nitrogen atom of aniline, diaminodiphenylmethane, isocyanuric acid, etc. is replaced with a glycidyl group; dicyclopentadiene type epoxy resins which are epoxidized from a copolymer resin of dicyclopentadiene and a phenol compound;Alicyclic epoxy resins such as vinylcyclohexene diepoxide, 3,4-epoxycyclohexylmethyl-3,4-epoxycyclohexanecarboxylate, and 2-(3,4-epoxy)cyclohexyl-5,5-spiro(3,4-epoxy)cyclohexane-m-dioxane, which have epoxidized olefin bonds within the molecule; paraxylylene-modified epoxy resins, which are glycidyl ethers of paraxylylene-modified phenol resins; metaxylylene-modified epoxy resins, which are glycidyl ethers of metaxylylene-modified phenol resins; terpene-modified epoxy resins, which are glycidyl ethers of terpene-modified phenol resins; and dicyclopentadiene-modified phenol resins, which are glycidyl ethers of dicyclo Examples of epoxy resins include: pentadiene-modified epoxy resins; cyclopentadiene-modified epoxy resins, which are glycidyl ethers of cyclopentadiene-modified phenolic resins; polycyclic aromatic ring-modified epoxy resins, which are glycidyl ethers of polycyclic aromatic ring-modified phenolic resins; naphthalene-type epoxy resins, which are glycidyl ethers of naphthalene ring-containing phenolic resins; halogenated phenol novolac-type epoxy resins; hydroquinone-type epoxy resins; trimethylolpropane-type epoxy resins; linear aliphatic epoxy resins obtained by oxidizing olefin bonds with peracids such as peracetic acid; and aralkyl-type epoxy resins, which are epoxidized aralkyl-type phenolic resins such as phenol aralkyl resins and naphthol aralkyl resins. Furthermore, epoxides of silicone resins and acrylic resins can also be cited as epoxy resins. These epoxy resins may be used individually or in combination of two or more types.

[0027] Among the epoxy resins mentioned above, epoxy resins selected from the group consisting of biphenyl-type epoxy resins, stilbene-type epoxy resins, diphenylmethane-type epoxy resins, sulfur atom-containing epoxy resins, novolac-type epoxy resins, dicyclopentadiene-type epoxy resins, triphenylmethane-type epoxy resins, copolymer-type epoxy resins, and aralkyl-type epoxy resins (these are referred to as "specific epoxy resins") from the viewpoint of balancing reflow resistance and fluidity. Specific epoxy resins may be used individually or in combination of two or more types.

[0028] When the epoxy resin contains a specific epoxy resin, from the viewpoint of exhibiting the performance of the specific epoxy resin, it is preferable that its total content be 30% by mass or more of the total epoxy resin, and more preferably 50% by mass or more.

[0029] Among specific epoxy resins, biphenyl-type epoxy resins, stilbene-type epoxy resins, diphenylmethane-type epoxy resins, and sulfur atom-containing epoxy resins are more preferred from the viewpoint of fluidity, and dicyclopentadiene-type epoxy resins, triphenylmethane-type epoxy resins, and aralkyl-type epoxy resins are preferred from the viewpoint of heat resistance.

[0030] In one embodiment, the epoxy resin preferably comprises at least one selected from the group consisting of aralkyl epoxy resins and biphenyl epoxy resins, and from the viewpoint of achieving both fluidity and heat resistance, it is more preferable to use aralkyl epoxy resins and biphenyl epoxy resins in combination.

[0031] When the epoxy resin contains an aralkyl epoxy resin, the content of the aralkyl epoxy resin is preferably 40% by mass or more of the total mass of the epoxy resin, more preferably 50% by mass or more, and even more preferably 60% by mass or more. Furthermore, the content of the aralkyl epoxy resin may be 100% by mass or less, 90% by mass or less, or 80% by mass or less of the total mass of the epoxy resin.

[0032] When the epoxy resin contains a biphenyl-type epoxy resin, the biphenyl-type epoxy resin content is preferably 5% by mass or more, preferably 10% by mass or more, and more preferably 20% by mass or more, of the total mass of the epoxy resin. Furthermore, the biphenyl-type epoxy resin content may be 60% by mass or less, 50% by mass or less, or 40% by mass or less, of the total mass of the epoxy resin.

[0033] When aralkyl epoxy resin and biphenyl epoxy resin are used in combination, the mass ratio (aralkyl epoxy resin:biphenyl epoxy resin) is preferably, for example, 40:60 to 95:5, more preferably 50:50 to 90:10, and even more preferably 60:40 to 80:20.

[0034] If the epoxy resin contains at least one selected from the group consisting of aralkyl epoxy resins and biphenyl epoxy resins, the total content of aralkyl epoxy resins and biphenyl epoxy resins relative to the total mass of the epoxy resin may be 50% by mass or more, 70% by mass or more, or 90% by mass or more.

[0035] The following are specific examples of preferred epoxy resins.

[0036] The biphenyl-type epoxy resin is not particularly limited as long as it is an epoxy resin having a biphenyl skeleton. For example, epoxy resins represented by the following general formula (II) are preferred. Among the epoxy resins represented by the following general formula (II), R 8 Of these, when the positions where the oxygen atom is substituted are designated as positions 4 and 4', the positions 3, 3', 5, and 5' are methyl groups, and the other R 8 YX-4000 and YX-4000H (Mitsubishi Chemical Corporation, product name), which are hydrogen atoms, all R 8 4,4'-bis(2,3-epoxypropoxy)biphenyl, where the hydrogen atom is, all R 8 When R is a hydrogen atom, and 8 Of these, when the positions where the oxygen atom is substituted are designated as positions 4 and 4', the positions 3, 3', 5, and 5' are methyl groups, and the other R 8 When the atom is a hydrogen atom, a mixed product such as YL-6121H (Mitsubishi Chemical Corporation, product name) is available commercially.

[0037] [ka]

[0038] In formula (II), R 8 represents a hydrogen atom, an alkyl group having 1 to 12 carbon atoms, or an aromatic group having 4 to 18 carbon atoms, and all of them may be the same or different. n is an average value and represents a number from 0 to 10.

[0039] The stilbene-type epoxy resin is not particularly limited as long as it is an epoxy resin having a stilbene skeleton. For example, an epoxy resin represented by the following general formula (III) is preferred. Among the epoxy resins represented by the following general formula (III), when the positions where oxygen atoms are substituted among R 9 are the 4- and 4'-positions, the 3,3',5,5'-positions are methyl groups, and the other R 9 is a hydrogen atom, and when all of R[[ID=eleven]] 10 are hydrogen atoms, and when three of the 3,3',5,5'-positions among R 9 are methyl groups and one is a t-butyl group, and the other R 9 is a hydrogen atom, and when all of R 10 are hydrogen atoms, a mixture such as ESLV-210 (Sumitomo Chemical Co., Ltd., trade name) is commercially available.

[0040]

Chemical formula

[0041] In formula (III), R 9 and R 10 represent a hydrogen atom or a monovalent organic group having 1 to 18 carbon atoms, and all of them may be the same or different. n is an average value and represents a number from 0 to 10.

[0042] The diphenylmethane-type epoxy resin is not particularly limited as long as it is an epoxy resin having a diphenylmethane skeleton. For example, an epoxy resin represented by the following general formula (IV) is preferred. Among the epoxy resins represented by the following general formula (IV), when all of R 11 are hydrogen atoms, and when the positions where oxygen atoms are substituted among R 12 are the 4- and​Products such as YSLV-80XY (Nippon Steel Chemical & Material Co., Ltd., product name), which contains a hydrogen atom, are available commercially.

[0043] [ka]

[0044] In formula (IV), R 11 and R 12 represents a hydrogen atom or a monovalent organic group with 1 to 18 carbon atoms, and these may all be the same or different. n is the average value and represents a number between 0 and 10.

[0045] Sulfur atom-containing epoxy resins are not particularly limited as long as they contain sulfur atoms. For example, epoxy resins represented by the following general formula (V) are included. Among the epoxy resins represented by the following general formula (V), R 13 Of these, when the positions where oxygen atoms are substituted are defined as positions 4 and 4', the 3,3' positions are t-butyl groups, the 6,6' positions are methyl groups, and the other R 13 Products such as YSLV-120TE (Nippon Steel Chemical & Material Co., Ltd., product name), which contains hydrogen atoms, are available commercially.

[0046] [ka]

[0047] In formula (V), R 13 represents a hydrogen atom or a monovalent organic group with 1 to 18 carbon atoms, and these may all be the same or different. n is the average value and represents a number between 0 and 10.

[0048] The novolac-type epoxy resin is not particularly limited as long as it is an epoxy resin obtained by epoxidizing a novolac-type phenolic resin. For example, epoxy resins obtained by epoxidizing novolac-type phenolic resins such as phenol novolac resin, cresol novolac resin, and naphthol novolac resin using methods such as glycidyl etherification are preferred, and epoxy resins represented by the following general formula (VI) are more preferred. Among the epoxy resins represented by the following general formula (VI), R 14 All of them are hydrogen atoms, R 15 The methyl group is i=1 in ESCN-190, ESCN-195 (Sumitomo Chemical Co., Ltd., product name), R 14 All of them are hydrogen atoms, i=0, N-770, N-775 (DIC Corporation, product name), R 14 All of them are hydrogen atoms, with parts where i=0 and parts where i=1, R 15 Styrene-modified phenol novolac type epoxy resins having a moiety that is -CH(CH3)-Ph, such as YDAN-1000-10C (Nippon Steel Chemical & Material Co., Ltd., product name), are commercially available.

[0049] [ka]

[0050] In formula (VI), R 14 R represents a hydrogen atom or a monovalent organic group having 1 to 18 carbon atoms, and these may all be the same or different. 15 '' represents a monovalent organic group with 1 to 18 carbon atoms, and each group may be identical or different. 'i' independently represents an integer from 0 to 3. 'n' is the average value, representing a number from 0 to 10.

[0051] The dicyclopentadiene type epoxy resin is not particularly limited as long as it is an epoxy resin obtained by epoxidizing a compound having a dicyclopentadiene skeleton as a raw material. For example, epoxy resins represented by the following general formula (VII) are preferred. Among the epoxy resins represented by the following general formula (VII), HP-7200 (DIC Corporation, trade name) where i=0 is available commercially.

[0052] [ka]

[0053] In formula (VII), R 16 '' represents a monovalent organic group with 1 to 18 carbon atoms, and each group may be identical or different. 'i' independently represents an integer from 0 to 3. 'n' is the average value, representing a number from 0 to 10.

[0054] The triphenylmethane-type epoxy resin is not particularly limited as long as it is an epoxy resin made from a compound having a triphenylmethane skeleton. For example, epoxy resins obtained by glycidyl etherification of triphenylmethane-type phenolic resins such as novolac-type phenolic resins made from a compound having a triphenylmethane skeleton and a compound having a phenolic hydroxyl group are preferred, and epoxy resins represented by the following general formula (VIII) are more preferred. Among the epoxy resins represented by the following general formula (VIII), 1032H60 (Mitsubishi Chemical Corporation, trade name) and EPPN-502H (Nippon Kayaku Co., Ltd., trade name), in which i is 0 and k is 0, are available commercially.

[0055] [ka]

[0056] In formula (VIII), R 17 and R 18 The '' represents a monovalent organic group with 1 to 18 carbon atoms, and each group may be identical or different. Each 'i' is an independent integer from 0 to 3, and each 'k' is an independent integer from 0 to 4. 'n' is the average value, representing a number from 0 to 10.

[0057] The copolymer epoxy resin obtained by epoxidizing a novolac resin obtained from a naphthol compound, a phenol compound, and an aldehyde compound is not particularly limited as long as it is an epoxy resin that uses compounds having a naphthol skeleton and compounds having a phenol skeleton as raw materials. For example, an epoxy resin obtained by glycidyl etherification of a novolac-type phenol resin using compounds having a naphthol skeleton and compounds having a phenol skeleton is preferred, and an epoxy resin represented by the following general formula (IX) is more preferred. Among the epoxy resins represented by the following general formula (IX), R 21 Products such as NC-7300 (Nippon Kayaku Co., Ltd., trade name), in which the group is a methyl group with i = 1, j = 0, and k = 0, are commercially available.

[0058] [ka]

[0059] In formula (IX), R 19 ~R 21 represents a monovalent organic group having 1 to 18 carbon atoms, and each group may be identical or different. i is an independent integer from 0 to 3, j is an independent integer from 0 to 2, and k is an independent integer from 0 to 4. l and m are average values, numbers from 0 to 10, and (l+m) is a number from 0 to 10. The end of the epoxy resin represented by formula (IX) is either formula (IX-1) or (IX-2) below. In formulas (IX-1) and (IX-2), R 19 ~R 21 The definitions of i, j and k are given by R in equation (IX). 19 ~R 21 The definitions of i, j, and k are the same. n is either 1 (when bonded via a methylene group) or 0 (when not bonded via a methylene group).

[0060] [ka]

[0061] Examples of epoxy resins represented by the above general formula (IX) include random copolymers containing l constituent units and m constituent units randomly, alternating copolymers containing units alternately, copolymers containing units regularly, and block copolymers containing units in a block-like manner. Any one of these may be used alone, or two or more may be used in combination.

[0062] As a copolymer epoxy resin, Epiclon HP-5000 (DIC Corporation, trade name), represented by the following general formula, is also preferred, as it is a methoxynaphthalene-cresol-formaldehyde cocondensation epoxy resin containing the following two structural units in a random, alternating, or block order. In the following general formula, n and m are each average values, numbers from 0 to 10, and (n+m) is a number from 0 to 10. Preferably, n and m are each average values, numbers from 1 to 9, and (n+m) is a number from 2 to 10.

[0063] [ka]

[0064] The aralkyl epoxy resin is not particularly limited as long as it is an epoxy resin made from a phenol resin synthesized from at least one selected from the group consisting of phenol compounds such as phenol and cresol and naphthol compounds such as naphthol and dimethylnaphthol, and dimethoxyparaxylene, bis(methoxymethyl)biphenyl, or derivatives thereof. For example, an epoxy resin obtained by glycidyl etherification of a phenol resin synthesized from at least one selected from the group consisting of phenol compounds such as phenol and cresol and naphthol compounds such as naphthol and dimethylnaphthol, and dimethoxyparaxylene, bis(methoxymethyl)biphenyl, or derivatives thereof is preferred, and epoxy resins represented by the following general formulas (X) and (XI) are more preferred.

[0065] Among the epoxy resins represented by the following general formula (X), i is 0 and R 38NC-3000S (Nippon Kayaku Co., Ltd., product name) has a hydrogen atom, i is 0, and R 38 Epoxy resins in which hydrogen atoms and all R of general formula (II) 8 Efficiency-based epoxy resins, such as CER-3000 (Nippon Kayaku Co., Ltd., trade name), which are mixed with an epoxy resin in which the θ is a hydrogen atom in a mass ratio of 80:20, are commercially available. In addition, among epoxy resins represented by the general formula (XI) below, ESN-175 (Nippon Steel Chemical & Material Co., Ltd., trade name), in which l is 0, j is 0, and k is 0, are commercially available.

[0066] [ka]

[0067] In equations (X) and (XI), R 38 R represents a hydrogen atom or a monovalent organic group having 1 to 18 carbon atoms, and these may all be the same or different. 37 , R 39 ~R 41 'i' represents a monovalent organic group with 1 to 18 carbon atoms, and each group may be identical or different. 'i' is an independent integer between 0 and 3, 'j' is an independent integer between 0 and 2, 'k' is an independent integer between 0 and 4, and 'l' is an independent integer between 0 and 6. 'n' is the average value, and each number is an independent number between 0 and 10.

[0068] In the above general formulas (II) to (XI), R 8 ~R 21 and R 37 ~R 41 Regarding this, "they may all be the same or all different" means, for example, the 8 to 88 R in equation (II) 8 This means that all of them may be the same or different. 9 ~R 21 and R 37 ~R 41 Regarding this as well, it means that the number of each element included in the formula may all be the same or different. Also, R 8 ~R 21 and R37 ~R 41 These can be the same or different. For example, R 9 and R 10 All of them may be the same or different. Furthermore, the monovalent organic group having 1 to 18 carbon atoms in general formulas (III) to (XI) is preferably an alkyl group or an aryl group.

[0069] In the above general formulas (II) to (XI), n is an average value, and it is preferable that each value is independently in the range of 0 to 10. When n is 10 or less, the melt viscosity of the resin component does not become too high, the viscosity of the epoxy resin composition during melt molding decreases, and the occurrence of filling defects, deformation of bonding wires (gold wires connecting the element and lead) tends to be suppressed. It is more preferable that n be set in the range of 0 to 4.

[0070] The epoxy equivalent of the epoxy resin is not particularly limited. From the viewpoint of balancing various properties such as moldability, reflow resistance, and electrical reliability, the epoxy equivalent of the epoxy resin is preferably 100 g / eq to 1000 g / eq, more preferably 150 g / eq to 500 g / eq, and even more preferably 160 g / eq to 300 g / eq. The epoxy equivalent of the epoxy resin shall be the value measured by the method in accordance with JIS K 7236:2009.

[0071] When the epoxy resin is solid, its softening point or melting 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 ease of handling during the preparation of the epoxy resin composition, it is more preferably 50°C to 130°C. The melting point of the epoxy resin shall be the value measured by differential scanning calorimetry (DSC), and the softening point of the epoxy resin shall be the value measured by the method (ring-ball method) in accordance with JIS K 7234:1986.

[0072] The epoxy resin content in the epoxy resin composition is preferably 0.5% to 50% by mass, and more preferably 2% to 30% by mass, from the viewpoint of strength, fluidity, heat resistance, moldability, etc.

[0073] <Phenol curing agent> The epoxy resin composition contains a phenol curing agent. Examples of phenol curing agents include phenol resins and polyhydric phenol compounds having two or more phenolic hydroxyl groups in one molecule. The phenol curing agent may be solid or liquid at 25°C and atmospheric pressure, but it is preferably solid. Specifically, a novolac-type phenolic resin obtained by condensing or co-condensing the above phenolic compounds with polyhydric phenol compounds such as resorcinol, catechol, bisphenol A, bisphenol F, and substituted or unsubstituted biphenols; at least one phenolic compound selected from the group consisting of phenol compounds such as phenol, m-cresol, p-cresol, xylenol, resorcinol, catechol, bisphenol A, bisphenol F, phenylphenol, aminophenol, and naphthol compounds such as α-naphthol, β-naphthol, and dihydroxynaphthalene, and an aldehyde compound such as formaldehyde, acetaldehyde, propionaldehyde, benzaldehyde, and salicylaldehyde under an acidic catalyst; and the above phenolic compounds with dimethoxyparaxylene, bis(methoxymethyl)bi Examples include aralkyl-type phenolic resins such as phenol aralkyl resins and naphthol aralkyl resins synthesized from phenyl and the like; paraxylylene and / or metaxylylene-modified phenolic resins; melamine-modified phenolic resins; terpene-modified phenolic resins; dicyclopentadiene-type phenolic resins and dicyclopentadiene-type naphthol resins synthesized by copolymerization of the above phenolic compounds and dicyclopentadiene; cyclopentadiene-modified phenolic resins; polycyclic aromatic ring-modified phenolic resins; biphenyl-type phenolic resins; triphenylmethane-type phenolic resins obtained by condensation or co-condensation of the above phenolic compounds with aromatic aldehyde compounds such as benzaldehyde and salicylaldehyde under an acidic catalyst; and phenolic resins obtained by copolymerizing two or more of these. These phenolic curing agents may be used individually or in combination of two or more.

[0074] Among phenol curing agents, at least one selected from the group consisting of aralkyl-type phenol resins, dicyclopentadiene-type phenol resins, triphenylmethane-type phenol resins, copolymerized phenol resins of benzaldehyde-type phenol resins and aralkyl-type phenol resins, and novolac-type phenol resins (these are referred to as "specific phenol curing agents") is preferred from the viewpoint of reflow resistance. Specific phenol curing agents may be used individually or in combination of two or more types.

[0075] In one embodiment, the phenol curing agent preferably contains an aralkyl-type phenol resin. The aralkyl-type phenol resin may be used in combination with other phenol curing agents. When the phenol resin contains an aralkyl-type phenol resin, the content of the aralkyl-type phenol resin may be 70% by mass or more, 80% by mass or more, or 90% by mass or more, based on the total mass of the phenol curing agent. The content of the aralkyl-type phenol resin may be 100% by mass or less, based on the total mass of the phenol curing agent.

[0076] The following are specific examples of preferred phenol curing agents.

[0077] Examples of aralkyl-type phenolic resins include phenolic aralkyl resins synthesized from phenolic compounds and dimethoxyp-xylene, bis(methoxymethyl)biphenyl, etc., and naphthol aralkyl resins. Aalkyl-type phenolic resins may be further copolymerized with other phenolic resins. Examples of copolymerized aralkyl-type phenolic resins include copolymerized phenolic resins of benzaldehyde-type phenolic resin and aralkyl-type phenolic resin, copolymerized phenolic resins of salicylaldehyde-type phenolic resin and aralkyl-type phenolic resin, and copolymerized phenolic resins of novolac-type phenolic resin and aralkyl-type phenolic resin.

[0078] The aralkyl-type phenolic resin is not particularly limited as long as it is synthesized from at least one compound selected from the group consisting of phenol compounds and naphthol compounds, and dimethoxyp-xylene, bis(methoxymethyl)biphenyl, or derivatives thereof. For example, phenolic resins represented by the following general formulas (XII) to (XIV) are preferred.

[0079] [ka]

[0080] In equations (XII) to (XIV), R 23 R represents a hydrogen atom or a monovalent organic group having 1 to 18 carbon atoms, and these may all be the same or different. 22 , R 24 , R 25 and R 28 R represents a monovalent organic group having 1 to 18 carbon atoms, and each of them may be identical or different. 26 and R 27 '' represents a hydroxyl group or a monovalent organic group having 1 to 18 carbon atoms, and each of these may be the same or different. 'i' is an independent integer between 0 and 3, 'j' is an independent integer between 0 and 2, 'k' is an independent integer between 0 and 4, and 'p' is an independent integer between 0 and 4. 'n' is the average value, and each of these is an independent number between 0 and 10.

[0081] Among the phenolic resins represented by the above general formula (XII), i is 0 and R 23 MEH-7851 (Meiwa Chemicals Co., Ltd., product name), which consists entirely of hydrogen atoms, is available commercially.

[0082] Among the phenolic resins represented by the above general formula (XIII), XL-225, XLC (Mitsui Chemicals, Inc., trade name), MEH-7800SS (Meiwa Kasei Co., Ltd., trade name), etc., in which i is 0 and k is 0, are available commercially.

[0083] Among the phenolic resins represented by the above general formula (XIV), SN-170 (Nippon Steel Chemical & Material Co., Ltd., product name) has j = 0, k = 0, and p = 0, while R has j = 0, k = 1. 27 SN-395 (Nippon Steel Chemical & Material Co., Ltd., product name), which has a hydroxyl group and p is 0, is available as a commercially available product.

[0084] The dicyclopentadiene-type phenolic resin is not particularly limited as long as it is a phenolic resin obtained from a compound having a dicyclopentadiene skeleton as a raw material. For example, a phenolic resin represented by the following general formula (XV) is preferred. Among the phenolic resins represented by the following general formula (XV), DPP (Shin Nippon Petrochemical Co., Ltd., trade name) in which i is 0 is available commercially.

[0085] [ka]

[0086] In formula (XV), R 29 '' represents a monovalent organic group with 1 to 18 carbon atoms, and each group may be identical or different. 'i' independently represents an integer from 0 to 3. 'n' is the average value, representing a number from 0 to 10.

[0087] The triphenylmethane-type phenolic resin is not particularly limited as long as it is a phenolic resin obtained from a compound having a triphenylmethane skeleton as a raw material. For example, a phenolic resin represented by the following general formula (XVI) is preferred.

[0088] Among the phenolic resins represented by the following general formula (XVI), MEH-7500 (Meiwa Chemicals Co., Ltd., product name), in which i is 0 and k is 0, is available commercially.

[0089] [ka]

[0090] In formula (XVI), R30 and R 31 '' represents a monovalent organic group with 1 to 18 carbon atoms, and each group may be identical or different. 'i' is an independent integer between 0 and 3, and 'k' is an independent integer between 0 and 4. 'n' is the average value, a number between 0 and 10.

[0091] The copolymerized phenol resin of a benzaldehyde-type phenol resin and an aralkyl-type phenol resin is not particularly limited as long as it is a copolymerized phenol resin of a phenol resin obtained from a compound having a benzaldehyde skeleton as a raw material and an aralkyl-type phenol resin. For example, a phenol resin represented by the following general formula (XVII) is preferred.

[0092] Among the phenolic resins represented by the following general formula (XVII), HE-510 (Air Water Chemical Co., Ltd., product name), in which i is 0, k is 0, and q is 0, is available commercially.

[0093] [ka]

[0094] In formula (XVII), R 32 ~R 34 represents a monovalent organic group with 1 to 18 carbon atoms, and each group may be identical or different. Each i is an independent integer from 0 to 3, each k is an independent integer from 0 to 4, and each q is an independent integer from 0 to 5. l and m are the average values, and each is an independent number from 0 to 11. However, the sum of l and m is a number from 1 to 11.

[0095] The novolac-type phenolic resin is not particularly limited as long as it is a phenolic resin obtained by condensing or co-condensing at least one phenolic compound selected from the group consisting of phenolic compounds and naphthol compounds with an aldehyde compound under an acidic catalyst. For example, a phenolic resin represented by the following general formula (XVIII) is preferred.

[0096] Among the phenolic resins represented by the following general formula (XVIII), those in which i is 0 and R 35 are all hydrogen atoms, such as Tamanol 758 and 759 (Arakawa Chemical Industries, Ltd., trade names), are available as commercial products.

[0097]

Chemical formula

[0098] In formula (XVIII), R 35 represents a hydrogen atom or a monovalent organic group having 1 to 18 carbon atoms, and they may all be the same or different from each other. R 36 represents a monovalent organic group having 1 to 18 carbon atoms, and they may all be the same or different from each other. i independently represents an integer of 0 to 3. n is an average value and represents a number of 0 to 10.

[0099] Regarding R 22 ~R 36 described in the above general formulas (XII) to (XVIII), "they may all be the same or different from each other" means that, for example, all of the i R 22 in formula (XII) may all be the same or different from each other. The same applies to the other R 23 ~R 36 , meaning that they may all be the same or different from each other for each number included in the formula. Also, R 22 ~R 36 may be the same or different from each other. For example, all of R 22 and R 23 may be the same or different from each other, and all of R 30 and R 31 may be the same or different from each other.

[0100] In the above general formulas (XII) to (XVIII), n is preferably in the range of 0 to 10. If it is 10 or less, the melt viscosity of the resin component will not become too high, the viscosity of the epoxy resin composition during melt molding will also be low, and defects in filling, deformation of bonding wires (gold wires connecting the element and lead) will be less likely to occur. The average n in one molecule is preferably set in the range of 0 to 4.

[0101] The hydroxyl group equivalent of the phenol curing agent is not particularly limited. From the viewpoint of balancing various properties such as moldability, 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.

[0102] The hydroxyl group equivalent of the phenol curing agent may be a value measured by, for example, a method in accordance with JIS K 0070:1992.

[0103] When the phenol curing agent is solid, its softening point or melting 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 ease of handling during the manufacture of the epoxy resin composition, it is more preferably 50°C to 130°C. Furthermore, from the viewpoint of improving fluidity and reducing the high-temperature modulus of the cured epoxy resin composition, thereby improving reflow resistance, the softening point or melting point of the phenol curing agent is preferably 50°C to 100°C, and more preferably 50°C to 75°C.

[0104] The melting point or softening point of the curing agent shall be a value measured in the same manner as the melting point or softening point of the epoxy resin.

[0105] The equivalent ratio of epoxy resin to phenol curing agent, i.e., the ratio of hydroxyl groups in the phenol curing agent to the number of epoxy groups in the epoxy resin (number of hydroxyl groups in phenol curing agent / number of epoxy groups in epoxy resin), is not particularly limited. From the viewpoint of minimizing unreacted components, the equivalent ratio of epoxy resin to phenol curing agent is preferably set in the range of 0.5 to 2.0, and more preferably in the range of 0.6 to 1.3. From the viewpoint of moldability and reflow resistance, it is even more preferable that the equivalent ratio of epoxy resin to phenol curing agent is set in the range of 0.8 to 1.2.

[0106] In the epoxy resin composition according to the first embodiment, the content of the phenol curing agent is 40 to 250 parts by mass per 100 parts by mass of epoxy resin. Preferably, the content of the phenol curing agent is 50 to 200 parts by mass, more preferably 60 to 170 parts by mass, even more preferably 70 to 140 parts by mass, and particularly preferably 80 to 125 parts by mass per 100 parts by mass of epoxy resin. In the epoxy resin composition according to the second embodiment, the content of the phenol curing agent is preferably 40 to 250 parts by mass, more preferably 50 to 200 parts by mass, even more preferably 60 to 170 parts by mass, particularly preferably 70 to 140 parts by mass, and most preferably 80 to 125 parts by mass per 100 parts by mass of epoxy resin. In a phenol-curable epoxy resin composition containing epoxy resin and phenol curing agent in the above proportions, it is presumed that the triazine ring-containing compound contributes favorably to the curing reaction and improves hygroscopic curability.

[0107] In the epoxy resin composition according to the first embodiment, the total mass of the epoxy resin and phenol curing agent relative to the total mass of tetrahydrofuran-soluble solids is preferably 85% by mass or more, more preferably 87% by mass or more, and even more preferably 89% by mass or more. In the epoxy resin composition according to the second embodiment, the total mass of the epoxy resin and phenol curing agent relative to the total mass of tetrahydrofuran-soluble solids is 85% by mass or more, preferably 87% by mass or more, and more preferably 89% by mass or more. In a phenol-curable epoxy resin composition containing epoxy resin and phenol curing agent in the above proportions, it is presumed that the triazine ring-containing compound contributes favorably to the curing reaction and improves hygroscopic curability.

[0108] In this disclosure, tetrahydrofuran-soluble solids refer to the soluble solids obtained when an epoxy resin composition is stirred and mixed with a sufficient amount of tetrahydrofuran at room temperature (e.g., 25°C). The mass of the tetrahydrofuran-soluble solids can be obtained by filtering the epoxy resin composition in which the soluble solids have been dissolved as described above. If the amounts of the components of the epoxy resin composition are known, the total amount of components soluble in tetrahydrofuran may be calculated under the above conditions.

[0109] The epoxy resin composition may also contain a curing agent other than a phenol curing agent in addition to the phenol curing agent. The proportion of the phenol curing agent to the total amount of curing agent is preferably 80% by mass or more, and preferably 90% by mass or more.

[0110] <Inorganic filler> The epoxy resin composition contains an inorganic filler. The material of the inorganic filler is not particularly limited. Specific examples of inorganic fillers include fused silica, crystalline silica, glass, alumina, calcium carbonate, zirconium silicate, calcium silicate, silicon nitride, aluminum nitride, boron nitride, magnesium oxide, silicon carbide, beryllia, zirconia, zircon, fossilite, steatite, spinel, mullite, titania, talc, clay, and mica. Inorganic fillers with flame-retardant properties may also be used. Examples of flame-retardant inorganic fillers include aluminum hydroxide, magnesium hydroxide, composite metal hydroxides such as magnesium-zinc composite hydroxides, and zinc borate. Among inorganic fillers, silica such as fused silica is preferred from the viewpoint of reducing the coefficient of thermal expansion, and alumina is preferred from the viewpoint of high thermal conductivity.

[0111] The shape of the inorganic filler is not particularly limited, but a spherical shape is preferred from the viewpoint of filling properties and mold wear resistance.

[0112] Inorganic fillers may be used individually or in combination of two or more types. "Using two or more inorganic fillers in combination" includes, for example, using two or more inorganic fillers with the same components but different average particle sizes, using two or more inorganic fillers with the same average particle size but different components, and using two or more inorganic fillers with different average particle sizes and types.

[0113] The content of inorganic fillers in the epoxy resin composition is not particularly limited. From the viewpoint of further improving properties such as the coefficient of thermal expansion, thermal conductivity, and elastic modulus of the cured product, the content of inorganic fillers is preferably 30% by volume or more of the total epoxy resin composition, more preferably 35% by volume or more, even more preferably 40% by volume or more, particularly preferably 45% by volume or more, and extremely preferably 50% by volume or more. From the viewpoint of improving fluidity and reducing viscosity, the content of inorganic fillers is preferably 99% by volume or less of the total epoxy resin composition, preferably 98% by volume or less, and more preferably 97% by volume or less. Furthermore, for example, when an epoxy resin composition is used for compression molding, the inorganic filler content may be 70% to 99% by volume of the total epoxy resin composition, 80% to 99% by volume, 83% to 99% by volume, or 85% to 99% by volume.

[0114] The inorganic filler content in the cured epoxy resin composition is measured as follows: First, the total mass of the cured material is measured. The cured material is then baked at 400°C for 2 hours, and then at 700°C for 3 hours to evaporate the resin components, and the mass of the remaining inorganic filler is measured. The volume is calculated from the obtained masses and their respective specific gravities, and the ratio of the volume of inorganic filler to the total volume of the cured material is obtained as the inorganic filler content.

[0115] The mass-based content of inorganic fillers in the epoxy resin composition may be 70% by mass or more, 80% by mass or more, or 85% by mass or more. Furthermore, the inorganic filler content in the epoxy resin composition may be 96% by mass or less, 95% by mass or less, or 94% by mass or less.

[0116] When the inorganic filler is particulate, its average particle size is not particularly limited. For example, the overall volume-average particle size of the inorganic filler is preferably 80 μm or less, but may also be 50 μm or less, 40 μm or less, 30 μm or less, 25 μm or less, 20 μm or less, or 15 μm. Furthermore, the overall volume-average particle size of the inorganic filler is preferably 0.1 μm or more, more preferably 0.2 μm or more, and even more preferably 0.3 μm or more. When the volume-average particle size of the inorganic filler is 0.1 μm or more, the increase in viscosity of the epoxy resin composition tends to be further suppressed. When the volume-average particle size is 80 μm or less, the ability to fill narrow gaps tends to be further improved. The volume-average particle size of the inorganic filler can be measured as the particle size (D50) when the cumulative amount from the small diameter side reaches 50% in the volume-based particle size distribution measured by a laser scattering diffraction particle size distribution analyzer.

[0117] <Triadine ring-containing compound> The epoxy resin composition contains a triazine ring-containing compound. In triazine ring-containing compounds, the position of nitrogen in the triazine ring is not particularly limited. That is, the triazine forming the backbone may be 1,2,3-triazine, 1,2,4-triazine, or 1,3,5-triazine. Among these, the triazine ring is preferably 1,3,5-triazine.

[0118] The molecular weight of the triazine ring-containing compound is not particularly limited and may be, for example, 100 to 800, 200 to 700, or 300 to 600.

[0119] In triazine ring-containing compounds, the triazine ring is preferably substituted. In particular, the triazine ring-containing compound is preferably substituted with a primary amino group or a secondary amino group, and more preferably with a primary amino group. That is, the triazine ring-containing compound is preferably substituted with a primary amino group in which at least one of the hydrogen atoms bonded to the three carbon atoms on triazine (C3H3N3) is substituted with a primary amino group. The substitution position of the monovalent group may be any of the three carbon atoms. The number of substitutions of the monovalent group may be one to three.

[0120] In one embodiment, the triazine ring-containing compound is preferably a compound represented by the following formula (I). The compound represented by the following formula (I) is presumed to have high compatibility with resin components and to be able to effectively exhibit properties such as moisture-absorbing curability, adhesion, and moisture resistance reliability.

[0121] [ka]

[0122] In formula (I), Y represents a monovalent organic group having 1 to 30 carbon atoms and containing a hydroxyl group, or a monovalent organic group having 1 to 30 carbon atoms and containing an alkoxysilyl group.

[0123] The number of carbon atoms in the organic group represented by Y is preferably 1 to 20, and more preferably 1 to 15.

[0124] In a preferred embodiment, the triazine ring-containing compound may be a compound represented by the following formula (II). The compound represented by the following formula (II) is presumed to have high compatibility with the resin component and to be able to effectively exhibit properties such as moisture-absorbing curability, adhesion, and moisture resistance reliability.

[0125] [ka]

[0126] In formula (II), each R independently represents a hydrogen atom, a hydroxyl group, a C1-C5 alkyl group, or a C1-C5 alkoxy group, and at least one of the three Rs is an alkoxy group. X represents a divalent linking group having 1-30 carbon atoms.

[0127] The C1-C5 alkyl group represented by R in formula (II) is preferably a methyl group or an ethyl group, and the C1-C5 alkoxy group is preferably a methoxy group or an ethoxy group.

[0128] The divalent linking group having 1 to 30 carbon atoms represented by X in formula (II) may be, for example, a hydrocarbon group, or a hydrocarbon group having heteroatoms such as a nitrogen atom or an oxygen atom. The length of the linking group, that is, the number of atoms on the atomic chain (excluding hydrogen atoms, branched chains, or substituents) between the silicon atom and the carbon atom on the triazine ring, may be 2 to 13 or 3 to 11.

[0129] The melting point of the triazine ring-containing compound is not particularly limited, but is preferably 200°C or lower, more preferably 175°C or lower, and even more preferably 150°C or lower. When the melting point of the triazine ring-containing compound is within the above range, the dispersibility of the triazine ring-containing compound increases, and properties such as adhesion tend to improve. In particular, a melting point of 150°C or lower is preferable because it increases dispersibility during kneading. From the viewpoint of handling and dispersibility, the melting point of the triazine ring-containing compound is preferably 0°C or higher, more preferably 10°C or higher, and even more preferably 25°C or higher. From the above viewpoint, the melting point of the triazine ring-containing compound is preferably 0°C to 200°C, more preferably 10°C to 175°C, and even more preferably 25°C to 150°C. The melting point of the triazine ring-containing compound can be measured by a melting point meter or the like.

[0130] From the viewpoint of moisture-absorbing curability and adhesion, the content of the triazine ring-containing compound relative to the total mass of the epoxy resin composition is preferably 0.3% by mass or more, more preferably 0.5% by mass or more, even more preferably 1.0% by mass or more, particularly preferably 2.0% by mass or more, and extremely preferably 3.0% by mass or more. Furthermore, the content of the triazine ring-containing compound relative to the total mass of the epoxy resin composition may be 20.0% by mass or less, 17.5% by mass or less, 15.0% by mass or less, 12.5% ​​by mass or less, or 10.0% by mass or less. When the content of the triazine ring-containing compound is within the above range, the elastic modulus tends to become excessively high, especially at high temperatures, and delamination between the internal components of the package and the sealing epoxy resin composition due to stress is suppressed. From the above viewpoint, the content of the triazine ring-containing compound relative to the total mass of the epoxy resin composition is preferably 0.3% to 20% by mass, more preferably 0.5% to 17.5% by mass, even more preferably 1.0% to 15.0% by mass, particularly preferably 2.0% to 12.5% ​​by mass, and extremely preferably 3.0% to 10.0% by mass.

[0131] <Various additives> In addition to the components described above, the epoxy resin composition may also contain various additives such as curing accelerators, coupling agents, ion exchangers, mold release agents, flame retardants, colorants, and stress relievers. The epoxy resin composition may also contain, as necessary, various additives well known in the art, in addition to those exemplified below.

[0132] (Curing accelerator) The epoxy resin composition may contain a curing accelerator. The type of curing accelerator is not particularly limited and can be selected according to the type of epoxy resin, the desired properties of the epoxy resin composition, etc. Examples of curing accelerators include diazabicycloalkenes such as 1,5-diazabicyclo[4.3.0]nonene-5 (DBN) and 1,8-diazabicyclo[5.4.0]undecene-7 (DBU); cyclic amidine compounds such as 2-methylimidazole, 2-phenylimidazole, 2-phenyl-4-methylimidazole, and 2-heptadecylimidazole; derivatives of the cyclic amidine compounds; phenol novolac salts of the cyclic amidine compounds or their derivatives; and quinone compounds such as maleic anhydride, 1,4-benzoquinone, 2,5-tholquinone, 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. Compounds having intramolecular polarization obtained by adding compounds with π bonds, such as zophenylmethane; cyclic amidinium compounds such as tetraphenylborate salt of DBU, tetraphenylborate salt of DBN, tetraphenylborate salt of 2-ethyl-4-methylimidazole, and tetraphenylborate salt of N-methylmorpholine; tertiary amine compounds such as pyridine, triethylamine, triethylenediamine, benzyldimethylamine, triethanolamine, dimethylaminoethanol, and tris(dimethylaminomethyl)phenol; derivatives of the above tertiary amine compounds; ammonium salt compounds such as tetra-n-butylammonium acetate, tetra-n-butylammonium phosphate, tetraethylammonium acetate, tetra-n-hexylammonium benzoate, and tetrapropylammonium hydroxide;Organic phosphines such as primary phosphines like ethylphosphine and phenylphosphine, secondary phosphines like dimethylphosphine and diphenylphosphine, triphenylphosphine, diphenyl(p-tolyl)phosphine, tris(alkylphenyl)phosphine, tris(alkoxyphenyl)phosphine, tris(alkyl·alkoxyphenyl)phosphine, tris(dialkylphenyl)phosphine, tris(trialkylphenyl)phosphine, tris(tetraalkylphenyl)phosphine, tris(dialkoxyphenyl)phosphine, tris(trialkoxyphenyl)phosphine, tris(tetraalkoxyphenyl)phosphine, trialkylphosphine, dialkylarylphosphine, alkyldiarylphosphine, trinaphthylphosphine, tris(benzyl)phosphine, and other tertiary phosphines; phosphine compounds such as complexes of the above organic phosphines with organoborons; and the above organic phosphines or the above phosphine compounds with maleic anhydride, 1,4-benzoquinone, 2,5-tholquinone, 1,4-naphthoquinone, 2,3-dimethylbenzox Compounds having intramolecular polarization obtained by adding compounds having π bonds, such as quinone compounds like 2,6-dimethylbenzoquinone, 2,3-dimethoxy-5-methyl-1,4-benzoquinone, 2,3-dimethoxy-1,4-benzoquinone, phenyl-1,4-benzoquinone, anthraquinone, and diazophenylmethane; and the aforementioned organophosphine or phosphine compound with 4-bromophenol, 3-bromophenol, 2-bromophenol, 4-chlorophenol, 3-chlorophenol, 2-chlorophenol, and 4-iodidepheno Compounds having intramolecular polarization obtained by reacting halogenated phenol compounds such as 3-iodidephenol, 2-iodidephenol, 4-bromo-2-methylphenol, 4-bromo-3-methylphenol, 4-bromo-2,6-dimethylphenol, 4-bromo-3,5-dimethylphenol, 4-bromo-2,6-di-t-butylphenol, 4-chloro-1-naphthol, 1-bromo-2-naphthol, 6-bromo-2-naphthol, and 4-bromo-4'-hydroxybiphenyl, followed by a dehalogenation step;Examples include tetrasubstituted phosphonium compounds such as tetraphenylphosphonium, tetraphenylborate salts of tetrasubstituted phosphoniums such as tetraphenylphosphonium tetra-p-tolylborate, and salts of tetrasubstituted phosphoniums with phenolic compounds; phosphobetaine compounds; and adducts of phosphonium compounds with silane compounds. The curing accelerator may be used alone or in combination of two or more types.

[0133] For example, particularly suitable curing accelerators when epoxy resin is used as the thermosetting resin include triphenylphosphine, and adducts of triphenylphosphine and quinone compounds.

[0134] When an epoxy resin composition contains a curing accelerator, the amount of the curing accelerator is preferably 0.1 to 10 parts by mass, more preferably 1 to 5 parts by mass, and even more preferably 1 to 3 parts by mass, per 100 parts by mass of the resin component (i.e., the total of the resin and the curing agent). When the amount of curing accelerator is 0.1 parts by mass or more per 100 parts by mass of the resin component, it tends to cure well in a short time. When the amount of curing accelerator is 10 parts by mass or less per 100 parts by mass of the resin component, it tends to result in a good molded product with a curing speed that is not too fast.

[0135] (Coupling agent) If the epoxy resin composition contains an inorganic filler, a coupling agent may be included to improve the adhesion between the resin component and the inorganic filler. In this disclosure, triazine ring-containing compounds are not included as coupling agents. Examples of known coupling agents include silane compounds such as epoxysilane, mercaptosilane, aminosilane, alkylsilane, ureidosilane, and vinylsilane, as well as titanium compounds, aluminum chelate compounds, and aluminum / zirconium compounds. In one embodiment, the epoxy resin composition is preferably made to include anilinosilane from the viewpoint of handling.

[0136] When the epoxy resin composition contains a coupling agent, the amount of the coupling agent is preferably 0.05 to 5 parts by mass, and more preferably 0.1 to 2.5 parts by mass, per 100 parts by mass of the inorganic filler. When the amount of the coupling agent is 0.05 parts by mass or more per 100 parts by mass of the inorganic filler, the adhesion to the frame tends to improve further. When the amount of the coupling agent is 5 parts by mass or less per 100 parts by mass of the inorganic filler, the moldability of the package tends to improve further.

[0137] From the viewpoint of adhesion between the resin component and the inorganic filler, it is preferable that the epoxy resin composition contains a silane coupling agent. Generally, silane coupling agents tend to adsorb moisture, and depending on the type and content of the silane coupling agent, this may cause an increase in water absorption. On the other hand, it has been found that the epoxy resin composition of this disclosure has excellent moisture-absorbing and curing properties even when it contains a silane coupling agent. From this viewpoint, when an epoxy resin composition contains a silane coupling agent, the content of the silane coupling agent may be 2.0% by mass or more, 3.0% by mass or more, or 3.5% by mass or more, based on the total mass of the resin components (for example, the total mass of the epoxy resin and the phenol curing agent). Furthermore, the content of the silane coupling agent may be 10.0% by mass or less, 8.0% by mass or less, or 6.0% by mass or less, based on the resin components.

[0138] (Ion exchanger) The epoxy resin composition may contain an ion exchanger. In particular, when the epoxy resin composition is used as a molding material for sealing, it is preferable to include an ion exchanger from the viewpoint of improving the moisture resistance and high-temperature storage characteristics of the electronic component device containing the element to be sealed. The ion exchanger is not particularly limited, and conventionally known ones 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. The ion exchanger may be used alone or in combination of two or more types.

[0139] When the epoxy resin composition contains an ion exchanger, its content is not particularly limited as long as it is sufficient to capture ions such as halogen ions. For example, it is preferably 0.1 parts by mass to 30 parts by mass, more preferably 1 part by mass to 15 parts by mass, based on 100 parts by mass of the resin component.

[0140] Among them, the epoxy resin composition preferably contains a hydrotalcite compound. The hydrotalcite compound has an anion exchange ability and captures ionic impurities such as chloride ions (Cl - ), formate ions (HCOO - ), acetate ions (CH3COO - ) mixed in the epoxy resin composition. Among them, the hydrotalcite compound has a high ability to capture chloride ions (Cl - ), and it is considered that by using it in combination with a triazine ring-containing compound in the epoxy resin composition, ionic impurities can be efficiently reduced and the moisture resistance reliability can be improved.

[0141] The hydrotalcite compound is a double salt compound containing magnesium, aluminum, hydroxyl groups, carbonate groups and optional water of crystallization. Further, in the above double salt compound, compounds in which a part of magnesium or aluminum is substituted with a metal such as an alkali metal or zinc; and compounds in which hydroxyl groups and carbonate groups are substituted with other anion groups are also mentioned as hydrotalcite compounds. Among them, hydrotalcite represented by the following general formula (A) is preferable.

[0142] Mg (1-X) Al X (OH)2(CO3) X / 2 ·mH2O ……(A) (0<X≦0.5, m is a positive number)

[0143] In formula (A), X is a positive number representing the substitution amount of Mg with Al, and it is preferably 0.20≦X≦0.33. m represents a positive number exceeding 0, and it is preferably 0<m≦2.

[0144] The hydrotalcite compound content is not particularly limited. From the viewpoint of improving moisture resistance reliability, the hydrotalcite compound content is preferably 0.5 parts by mass or more, more preferably 0.8 parts by mass or more, and even more preferably 1.0 part by mass or more, per 100 parts by mass of epoxy resin. From the viewpoint of fully exhibiting the effects of other components, and from the viewpoint of suppressing the decrease in filling ability into narrow sections and wire flow due to viscosity increase, the hydrotalcite compound content is preferably 20.0 parts by mass or less, more preferably 15.0 parts by mass or less, and even more preferably 10.0 parts by mass or less, per 100 parts by mass of epoxy resin. From the above viewpoint, the hydrotalcite compound content is preferably 0.5 to 20.0 parts by mass, more preferably 0.8 to 15.0 parts by mass, and even more preferably 1.0 to 10.0 parts by mass, per 100 parts by mass of epoxy resin.

[0145] Furthermore, the hydrotalcite compound content may be 3.0 parts by mass or less, 2.0 parts by mass or less, or 1.5 parts by mass or less per 100 parts by mass of epoxy resin, from the viewpoint of fully exhibiting the effects of other components and from the viewpoint of suppressing the reduction in filling ability into narrow sections and wire flow due to thickening. In the epoxy resin compositions according to the first and second embodiments, ionic impurities can be suitably reduced even if the hydrotalcite content is kept within the above range. The hydrotalcite content may be 0.1 to 3.0 parts by mass, 0.2 to 2.0 parts by mass, or 0.3 to 1.5 parts by mass per 100 parts by mass of epoxy resin.

[0146] (Release agent) The epoxy resin composition may contain a release agent to obtain good release properties from the mold during molding. The release agent is not particularly limited, and conventionally known ones can be used. Specifically, examples include carnauba wax, higher fatty acids such as montanic acid and stearic acid, higher fatty acid metal salts, ester waxes such as montanic acid esters, and polyolefin waxes such as oxidized polyethylene and non-oxidized polyethylene. The release agent may be used alone or in combination of two or more types.

[0147] When the epoxy resin composition contains a release agent, the amount is preferably 0.01 to 15 parts by mass, and more preferably 0.1 to 10 parts by mass, per 100 parts by mass of the resin component. When the amount of release agent is 0.01 parts by mass or more per 100 parts by mass of the resin component, sufficient release properties tend to be obtained. When it is 15 parts by mass or less, better adhesion tends to be obtained.

[0148] (Flame retardant) The epoxy resin composition may contain a flame retardant. The flame retardant is not particularly limited, and conventionally known ones can be used. Specifically, examples include organic or inorganic compounds containing halogen atoms, antimony atoms, nitrogen atoms, or phosphorus atoms, and metal hydroxides. The flame retardant may be used alone or in combination of two or more types.

[0149] If the epoxy resin composition contains a flame retardant, the amount is not particularly limited as long as it is sufficient to obtain the desired flame retardant effect. For example, it is preferably 1 to 300 parts by mass, and more preferably 2 to 150 parts by mass, per 100 parts by mass of the resin component.

[0150] (Coloring agent) The epoxy resin composition may further contain a coloring agent. Examples of known coloring agents include carbon black, organic dyes, organic pigments, titanium dioxide, red lead, and red iron oxide. The amount of coloring agent can be appropriately selected depending on the purpose. The coloring agent may be used alone or in combination of two or more types.

[0151] (Stress reliever) The epoxy resin composition may contain stress-relieving agents such as silicone oil and silicone rubber particles. Including stress-relieving agents can further reduce package warping and the occurrence of package cracks. Examples of commonly used stress-relieving agents (flexible agents) include thermoplastic elastomers such as silicone-based, styrene-based, olefin-based, urethane-based, polyester-based, polyether-based, polyamide-based, and polybutadiene-based agents; rubber particles such as NR (natural rubber), NBR (acrylonitrile-butadiene rubber), acrylic rubber, urethane rubber, and silicone powder; and rubber particles having a core-shell structure such as methyl methacrylate-styrene-butadiene copolymer (MBS), methyl methacrylate-silicone copolymer, and methyl methacrylate-butyl acrylate copolymer. One type of stress-relieving agent may be used alone, or two or more types may be used in combination. Among these, silicone-based stress-relieving agents are preferred. Examples of silicone-based stress-relieving agents include those having epoxy groups, those having amino groups, and those modified with polyether.

[0152] [Method for preparing epoxy resin compositions] The method for preparing the epoxy resin composition is not particularly limited. A common method involves thoroughly mixing predetermined amounts of components using a mixer or the like, then melt-kneading them using a mixing roll, extruder, or the like, followed by cooling and pulverization. More specifically, for example, a method involves uniformly stirring and mixing predetermined amounts of the above-mentioned components, then kneading them using a kneader, roll, extruder, or the like that has been preheated to 70°C to 140°C, followed by cooling and pulverization.

[0153] The epoxy resin composition is preferably solid at room temperature and atmospheric pressure (for example, 25°C and atmospheric pressure). The shape of the epoxy resin composition when it is solid is not particularly limited, and examples include powder, granules, and tablets. When the epoxy resin composition is in tablet form, the dimensions and mass are preferably such that they are suitable for the packaging molding conditions, from the viewpoint of ease of handling.

[0154] [Uses of epoxy resin compositions] The epoxy resin composition is used for sealing the element. The method of sealing the element is not particularly limited and may be a transfer molding method, injection molding method, compression molding method, etc.

[0155] [Properties of epoxy resin compositions and their cured products] (moisture curability) The epoxy resin composition exhibits excellent moisture-absorbing and curing properties. Moisture-absorbing and curing properties can be evaluated by the following method. The powdered epoxy resin composition is placed in a constant temperature and humidity chamber at 25°C and 50% RT and stored for a predetermined time (e.g., 24 hours, 48 ​​hours, or 74 hours). After each time period, each epoxy resin composition is removed from the constant temperature and humidity chamber and molded in a transfer molding machine under the conditions of a mold temperature of 180°C, a molding pressure of 6.9 MPa, and a molding time of 90 seconds to prepare test specimens. The hot hardness of each cured product is measured using a Shore D hardness tester (e.g., Ueshima Seisakusho Co., Ltd., HD-1120 (Type D)). Moisture-absorbing curing properties can be measured specifically by the method described in the examples.

[0156] The thermal hardness of an epoxy resin composition stored in a constant temperature and humidity chamber for 72 hours under the above conditions is preferably 80% or more, and more preferably 85% or more, than the thermal hardness of a cured epoxy resin composition that was not stored in a constant temperature and humidity chamber.

[0157] (Water absorption rate of hardened material) The water absorption rate of the cured epoxy resin composition is preferably 1.00% by mass or less, preferably 0.80% by mass or less, and preferably 0.50% by mass or less. A lower water absorption rate is preferable, but the water absorption rate of the cured epoxy resin composition may be 0.10% by mass or more, preferably 0.20% by mass or more, and may be 0.30% by mass or more.

[0158] The water absorption rate is defined as the mass increase rate obtained by the following formula when the cured product is left at 121°C and 2 atmospheres for 20 hours. The water absorption rate can be specifically measured by the method described in the examples. Water absorption rate (mass %) = {(Amount of hardened material after standing - Amount of hardened material before standing) / Amount of hardened material before standing} × 100

[0159] When evaluating the water absorption rate of a cured epoxy resin composition, the water absorption rate of the cured product is measured using a transfer molding machine, molded under the conditions of a mold temperature of 180°C, a molding pressure of 6.9 MPa, and a molding time of 90 seconds, and cured at 175°C for 5 hours.

[0160] The water absorption rate of an epoxy resin composition can be adjusted, for example, by adjusting the equivalent amount of epoxy resin. Increasing the epoxy equivalent amount of epoxy resin tends to lower the crosslinking density of the cured product, thus lowering the water absorption rate. Furthermore, the water absorption rate can also be adjusted by controlling the type and amount of each component, such as silane coupling agents and inorganic fillers.

[0161] <Epoxy resin compositions for sealing according to the third and fourth embodiments> The epoxy resin composition for sealing according to the third embodiment of this disclosure contains an epoxy resin, a phenol curing agent, an inorganic filler, a triazine ring-containing compound, and a hydrotalcite compound, wherein the content of the phenol curing agent is 40 to 250 parts by mass per 100 parts by mass of the epoxy resin.

[0162] The epoxy resin composition for sealing according to the fourth embodiment of this disclosure contains an epoxy resin, a phenol curing agent, an inorganic filler, a triazine ring-containing compound, and a hydrotalcite compound, wherein the total mass of the epoxy resin and the phenol curing agent is 85% by mass or more with respect to the total mass of tetrahydrofuran-soluble solids in the epoxy resin composition for sealing.

[0163] The epoxy resin compositions according to the third and fourth embodiments make it possible to manufacture electronic component devices with excellent moisture resistance reliability. The reason for this is presumed to be as follows: Through the inventors' studies, it was found that the triazine-containing compound has the effect of reducing the content of ionic impurities, particularly organic acid ions, in the extract of the epoxy resin composition. It is thought that this effect of reducing organic acid ions, combined with the ion capture effect of the hydrotalcite compound, can efficiently reduce the content of ionic impurities. As a result, it is thought that the electrical conductivity in the extract can be reduced, and the moisture resistance reliability of the electronic component device can be improved.

[0164] Furthermore, in one embodiment, it has been found that the epoxy resin compositions according to the third and fourth embodiments tend to exhibit excellent moisture-absorbing curing properties. Although the reason for this is not clear, it is presumed that one reason is that the triazine ring-containing compound contributes to the reaction between the epoxy resin and the phenol curing agent, thereby suppressing the decrease in curability due to moisture absorption in the epoxy resin composition. In addition, in one embodiment, it has been found that the epoxy resin compositions according to the third and fourth embodiments tend to exhibit excellent adhesion to metals such as copper and silver. It is thought that the nitrogen atoms in the triazine ring of the triazine ring-containing compounds contribute to the adhesion to metals. Due to these properties, the epoxy resin compositions according to the third and fourth embodiments are considered suitable for use in the manufacture of highly moisture-resistant electronic component devices.

[0165] The epoxy resin compositions according to the third and fourth embodiments may further contain additives and the like. The components that may be included in the epoxy resin compositions according to the third and fourth embodiments will be described in detail below.

[0166] <Epoxy resin> Details and preferred embodiments of the epoxy resin can be applied to the details and preferred embodiments of the epoxy resin contained in the epoxy resin composition according to the first and second embodiments.

[0167] <Phenol curing agent> Details and preferred embodiments of the phenol curing agent can be applied to the details and preferred embodiments of the phenol curing agent contained in the epoxy resin composition according to the first and second embodiments.

[0168] In the epoxy resin composition according to the third embodiment, the content of the phenol curing agent is 40 to 250 parts by mass per 100 parts by mass of epoxy resin. Preferably, the content of the phenol curing agent is 50 to 200 parts by mass, more preferably 60 to 170 parts by mass, even more preferably 70 to 140 parts by mass, and particularly preferably 80 to 125 parts by mass per 100 parts by mass of epoxy resin. In the epoxy resin composition according to the fourth embodiment, the content of the phenol curing agent is preferably 40 to 250 parts by mass, more preferably 50 to 200 parts by mass, even more preferably 60 to 170 parts by mass, particularly preferably 70 to 140 parts by mass, and most preferably 80 to 125 parts by mass, per 100 parts by mass of epoxy resin.

[0169] In the epoxy resin composition according to the third embodiment, the total mass of the epoxy resin and phenol curing agent relative to the total mass of tetrahydrofuran-soluble solids is preferably 85% by mass or more, more preferably 87% by mass or more, and even more preferably 89% by mass or more. In the epoxy resin composition according to the fourth embodiment, the total mass of the epoxy resin and phenol curing agent relative to the total mass of tetrahydrofuran-soluble solids is 85% by mass or more, preferably 87% by mass or more, and more preferably 89% by mass or more.

[0170] <Inorganic filler> Details and preferred embodiments of the inorganic filler can be applied to the details and preferred embodiments of the inorganic filler contained in the epoxy resin composition according to the first and second embodiments.

[0171] <Triadine ring-containing compound> The epoxy resin composition contains a triazine ring-containing compound. In triazine ring-containing compounds, the position of nitrogen in the triazine ring is not particularly limited. That is, the triazine forming the backbone may be 1,2,3-triazine, 1,2,4-triazine, or 1,3,5-triazine. Among these, the triazine ring is preferably 1,3,5-triazine.

[0172] The molecular weight of the triazine ring-containing compound is not particularly limited and may be, for example, 100 to 800, 200 to 700, or 300 to 600.

[0173] In triazine ring-containing compounds, the triazine ring is preferably substituted. In particular, the triazine ring-containing compound is preferably substituted with a primary amino group or a secondary amino group, and more preferably with a primary amino group. That is, the triazine ring-containing compound is preferably substituted with a primary amino group in which at least one of the hydrogen atoms bonded to the three carbon atoms on triazine (C3H3N3) is substituted with a primary amino group. The substitution position of the monovalent group may be any of the three carbon atoms. The number of substitutions of the monovalent group may be one to three.

[0174] In one embodiment, the triazine ring-containing compound is preferably a compound represented by the following formula (I). The compound represented by the following formula (I) is presumed to have high compatibility with resin components and to be able to effectively exhibit properties such as moisture resistance reliability, moisture curing properties, and adhesive properties.

[0175] [ka]

[0176] In formula (I), Y represents a monovalent organic group having 1 to 30 carbon atoms and containing a hydroxyl group, or a monovalent organic group having 1 to 30 carbon atoms and containing an alkoxysilyl group.

[0177] The number of carbon atoms in the organic group represented by Y is preferably 1 to 20, and more preferably 1 to 15.

[0178] In a preferred embodiment, the triazine ring-containing compound may be a compound represented by the following formula (II). The compound represented by the following formula (II) is presumed to have high compatibility with the resin component and to be able to effectively exhibit properties such as moisture resistance reliability, moisture curing properties, and adhesive properties.

[0179] [ka]

[0180] In formula (II), each R independently represents a hydrogen atom, a hydroxyl group, a C1-C5 alkyl group, or a C1-C5 alkoxy group, and at least one of the three Rs is an alkoxy group. X represents a divalent linking group having 1-30 carbon atoms.

[0181] The C1-C5 alkyl group represented by R in formula (II) is preferably a methyl group or an ethyl group, and the C1-C5 alkoxy group is preferably a methoxy group or an ethoxy group.

[0182] The divalent linking group having 1 to 30 carbon atoms represented by X in formula (II) may be, for example, a hydrocarbon group, or a hydrocarbon group having heteroatoms such as a nitrogen atom or an oxygen atom. The length of the linking group, that is, the number of atoms on the atomic chain (excluding hydrogen atoms, branched chains, or substituents) between the silicon atom and the carbon atom on the triazine ring, may be 2 to 13 or 3 to 11.

[0183] The melting point of the triazine ring-containing compound is not particularly limited, but is preferably 200°C or lower, more preferably 175°C or lower, and even more preferably 150°C or lower. When the melting point of the triazine ring-containing compound is within the above range, the dispersibility of the triazine ring-containing compound increases, and properties such as adhesion tend to improve. In particular, a melting point of 150°C or lower is preferable because it increases dispersibility during kneading. From the viewpoint of handling and dispersibility, the melting point of the triazine ring-containing compound is preferably 0°C or higher, more preferably 10°C or higher, and even more preferably 25°C or higher. From the above viewpoint, the melting point of the triazine ring-containing compound is preferably 0°C to 200°C, more preferably 10°C to 175°C, and even more preferably 25°C to 150°C. The melting point of the triazine ring-containing compound can be measured by a melting point meter or the like.

[0184] From the viewpoint of moisture resistance reliability, the content of the triazine ring-containing compound relative to the total mass of the epoxy resin composition is preferably 0.3% by mass or more, and more preferably 0.5% by mass or more. Furthermore, the content of the triazine ring-containing compound relative to the total mass of the epoxy resin composition may be 10.0% by mass or less, 8.0% by mass or less, 6.0% by mass or less, or 5.0% by mass or less. When the content of the triazine ring-containing compound is within the above range, the elastic modulus tends to become excessively high, especially at high temperatures, and delamination between the internal components of the package and the sealing epoxy resin composition due to stress is suppressed. From the above viewpoint, the content of the triazine ring-containing compound relative to the total mass of the epoxy resin composition is preferably 0.3% to 10.0% by mass, more preferably 0.5% to 8.0% by mass, even more preferably 0.5% to 6.0% by mass, and particularly preferably 0.5% to 5.0% by mass.

[0185] Furthermore, from the viewpoint of moisture-absorbing curability and adhesion, the content of the triazine ring-containing compound relative to the total mass of the epoxy resin composition is preferably 0.3% by mass or more, more preferably 0.5% by mass or more, even more preferably 1.0% by mass or more, particularly preferably 2.0% by mass or more, and extremely preferably 3.0% by mass or more. Furthermore, the content of the triazine ring-containing compound relative to the total mass of the epoxy resin composition may be 20.0% by mass or less, 17.5% by mass or less, 15.0% by mass or less, 12.5% ​​by mass or less, or 10.0% by mass or less. When the content of the triazine ring-containing compound is within the above range, the elastic modulus tends to become excessively high, especially at high temperatures, and delamination between the internal components of the package and the sealing epoxy resin composition due to stress is suppressed. From the above viewpoint, the content of the triazine ring-containing compound relative to the total mass of the epoxy resin composition is preferably 0.3% to 20% by mass, more preferably 0.5% to 17.5% by mass, even more preferably 1.0% to 15.0% by mass, particularly preferably 2.0% to 12.5% ​​by mass, and extremely preferably 3.0% to 10.0% by mass.

[0186] <Hydrotalcite compounds> The epoxy resin composition contains a hydrotalcite compound. The hydrotalcite compound has anion exchange ability and contains chloride ions (Cl) present in the epoxy resin composition. - ), formate ions (HClO - ), acetate ion (CH3COO -) captures ionic impurities such as. Among them, hydrotalcite compounds have a high ability to capture chloride ions (Cl - ), and it is considered that ionic impurities can be efficiently reduced by using them in combination with a triazine ring-containing compound.

[0187] A hydrotalcite compound is a double salt compound containing magnesium, aluminum, hydroxyl groups, carbonate groups and optional water of crystallization. Further, in the above double salt compound, compounds in which a part of magnesium or aluminum is substituted with a metal such as an alkali metal or zinc; and compounds in which hydroxyl groups and carbonate groups are substituted with other anion groups are also mentioned as hydrotalcite compounds. Among them, hydrotalcite represented by the following general formula (A) is preferable.

[0188] Mg (1-X) Al X (OH)2(CO3) X / 2 ·mH2O ……(A) (0 < X ≦ 0.5, m is a positive number)

[0189] In formula (A), X is a positive number representing the substitution amount of Mg with Al, and it is preferably 0.20 ≦ X ≦ 0.33. m represents a positive number exceeding 0, and it is preferably 0 < m ≦ 2.

[0190] The hydrotalcite compound may be a natural product or a synthetic product. Also, the hydrotalcite compound may be an uncalcined hydrotalcite compound or a calcined hydrotalcite compound, or an uncalcined hydrotalcite compound and a calcined hydrotalcite compound may be used in combination. Examples of the uncalcined hydrotalcite compound include the uncalcined compound represented by the above formula (A), and examples of the calcined hydrotalcite compound include the calcined product of the compound represented by the above formula (A).

[0191] Hydrotalcite compounds may be used individually or in combination of two or more. When using two or more hydrotalcite compounds, examples include using two or more compounds with different Mg / Al ratios, average particle sizes, specific surface areas, calcination conditions, etc.

[0192] The shape of the hydrotalcite compound is not particularly limited, but it is preferably particulate. When the hydrotalcite compound is particulate, the average particle size is not particularly limited. From the viewpoint of fluidity, the hydrotalcite compound is preferably particulate, with a volume average particle size of 0.01 μm to 15 μm, more preferably 0.1 μm to 5 μm, and even more preferably 0.1 μm to 1 μm. When the hydrotalcite compound is in the state of secondary particles, the above volume average particle size represents the volume average particle size of the secondary particles. The volume-average particle size of hydrotalcite compounds can be measured as the particle size (D50) at which the cumulative amount from the smaller diameter side reaches 50% in the volume-based particle size distribution measured by a laser scattering diffraction particle size distribution analyzer.

[0193] Furthermore, the epoxy resin composition preferably contains a hydrotalcite compound with a volume-average particle diameter of 0.6 μm or less, and more preferably contains a hydrotalcite compound with a volume-average particle diameter of 0.1 μm to 0.6 μm. When the epoxy resin composition contains a hydrotalcite compound with a volume-average particle diameter of 0.6 μm or less, burrs tend to be suppressed during molding.

[0194] The specific surface area of ​​the hydrotalcite compound is not particularly limited, 1 m 2 It is preferable that it is 5m or more per gram. 2 It is more preferable that it be 10m or more per gram. 2 It is even more preferable that the amount be 100 m² or more. There is no particular upper limit to the specific surface area of ​​the hydrotalcite compound, up to 100 m². 2 It may also be / g. In this disclosure, the specific surface area of ​​the hydrotalcite compound shall be the value measured by the BET method.

[0195] The hydrotalcite compound content is not particularly limited. From the viewpoint of improving moisture resistance reliability, the hydrotalcite compound content is preferably 0.5 parts by mass or more, more preferably 0.8 parts by mass or more, and even more preferably 1.0 part by mass or more, per 100 parts by mass of epoxy resin. From the viewpoint of fully exhibiting the effects of other components, and from the viewpoint of suppressing the decrease in filling ability into narrow sections and wire flow due to viscosity increase, the hydrotalcite compound content is preferably 20.0 parts by mass or less, more preferably 15.0 parts by mass or less, and even more preferably 10.0 parts by mass or less, per 100 parts by mass of epoxy resin. From the above viewpoint, the hydrotalcite compound content is preferably 0.5 to 20.0 parts by mass, more preferably 0.8 to 15.0 parts by mass, and even more preferably 1.0 to 10.0 parts by mass, per 100 parts by mass of epoxy resin.

[0196] Furthermore, from the viewpoint of fully exhibiting the effects of other components, and from the viewpoint of suppressing the decrease in filling ability into narrow sections and wire flow due to increased viscosity, the hydrotalcite compound content may be 3.0 parts by mass or less, 2.0 parts by mass or less, or 1.5 parts by mass or less per 100 parts by mass of epoxy resin. In the epoxy resin compositions according to the third and fourth embodiments, ionic impurities can be suitably reduced even if the hydrotalcite content is kept within the above range. The hydrotalcite content may be 0.1 to 3.0 parts by mass, 0.2 to 2.0 parts by mass, or 0.3 to 1.5 parts by mass per 100 parts by mass of epoxy resin.

[0197] <Various additives> In addition to the components described above, the epoxy resin composition may also contain various additives such as curing accelerators, coupling agents, ion exchangers other than hydrotalcite compounds, mold release agents, flame retardants, colorants, and stress relievers. The epoxy resin composition may also contain, as necessary, various additives well known in the art, in addition to the additives exemplified below.

[0198] Details and preferred embodiments of the curing accelerator, coupling agent, mold release agent, flame retardant, coloring agent, and stress reliever can be applied to the details and preferred embodiments of each component included in the epoxy resin composition according to the first and second embodiments.

[0199] (Ion exchanger) The epoxy resin composition may or may not contain an ion exchanger other than the hydrotalcite compound. Examples of the ion exchanger other than the hydrotalcite compound include metal hydroxides such as those containing at least one element selected from the group consisting of magnesium, aluminum, titanium, zirconium, and bismuth. The ion exchanger may be used alone or in combination of two or more.

[0200] When the epoxy resin composition contains an ion exchanger, its content is not particularly limited as long as it is sufficient to capture ions such as halogen ions. For example, it is preferably 0.1 to 30 parts by mass, more preferably 1 to 15 parts by mass, based on 100 parts by mass of the resin component.

[0201] [Method for preparing epoxy resin composition] The method for preparing the epoxy resin composition is not particularly limited. As a general method, there can be mentioned a method in which components in predetermined blending amounts are sufficiently mixed by a mixer or the like, and then melt-kneaded by a mixing roll, an extruder or the like, cooled, and pulverized. More specifically, for example, there can be mentioned a method in which a predetermined amount of the above-described components are uniformly stirred and mixed, and kneaded by a kneader, a roll, an extruder or the like that has been preheated to 70°C to 140°C, cooled, and pulverized.

[0202] The epoxy resin composition is preferably solid at normal temperature and pressure (for example, 25°C, atmospheric pressure). The shape of the epoxy resin composition when it is solid is not particularly limited, and examples include powder form, granular form, tablet form, etc. From the viewpoint of handling properties, when the epoxy resin composition is in tablet form, the dimensions and mass are preferably such that they match the molding conditions of the package.

[0203] 〔Use of the epoxy resin composition〕 The epoxy resin composition is used for encapsulating elements. The method for encapsulating the elements is not particularly limited, and it may be a transfer molding method, an injection molding method, a compression molding method, etc.

[0204] 〔Properties of the epoxy resin composition and its cured product〕 (Moisture resistance reliability) The moisture resistance reliability can be evaluated using the electrical conductivity of the extract of the epoxy resin composition as an index. The electrical conductivity of the extract is measured, for example, as follows. 50 g of ion-exchanged water and 5 g of the pulverized powder of the prepared epoxy resin composition are put into a pressure-resistant container, left for 20 hours at 121°C and 2 atm to obtain an extract. Measure the electrical conductivity of the extract. The lower the electrical conductivity of the extract obtained by the above procedure, the more preferable it is. From the viewpoint of moisture resistance reliability, it is preferably 100 μS / cm or less, more preferably 90 μS / cm or less, further preferably 80 μS / cm or less, particularly preferably 70 μS / cm or less, and extremely preferably 60 μS / cm or less.

[0205] (Content of ionic impurities in the extract) From the viewpoint of suppressing the corrosion of metal members such as wires in an electronic component device and enhancing the moisture resistance reliability, the content of ionic impurities in the extract of the epoxy resin composition is preferably as low as possible. The content of ionic impurities in the epoxy resin composition can be determined as follows. 50 g of deionized water and 5 g of pulverized epoxy resin powder prepared were placed in a pressure vessel, and after standing at 121°C and 2 atmospheres for 20 hours, the ion concentration of the extract was measured using ion chromatography. The chloride ions (Cl) measured using the above procedure - The content of ) is preferably 20 ppm or less, more preferably 15 ppm or less, and even more preferably 10 ppm or less. The formate ions (HClO) measured using the above procedure - The content of ) is preferably 100 ppm or less, more preferably 90 ppm or less, and even more preferably 80 ppm or less. The acetate ion (CH3COO) measured using the above procedure - The content of ) is preferably 70 ppm or less, more preferably 60 ppm or less, and even more preferably 50 ppm or less.

[0206] ≪Electronic Components and Equipment≫ An electronic component device according to one aspect of the present disclosure comprises an element and a cured product of an epoxy resin composition selected from the first to fourth embodiments described above for sealing the element. Examples of electronic component devices include those in which elements (active elements such as semiconductor chips, transistors, diodes, and thyristors, and passive elements such as capacitors, resistors, and coils) are mounted on support members such as lead frames, pre-wired tape carriers, wiring boards, glass, silicon wafers, and organic substrates, and the resulting element section is sealed with an epoxy resin composition. More specifically, common resin-encapsulated ICs such as 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) have a structure in which elements are fixed on a lead frame, the terminal parts of the elements such as bonding pads are connected to the lead parts by wire bonding, bumps, etc., and then sealed using an epoxy resin composition by transfer molding, etc.; TCP (Tape Carrier Package) has a structure in which elements connected to a tape carrier by bumps are sealed with an epoxy resin composition; and COB (Chip On) has a structure in which elements connected to wiring formed on a support member by wire bonding, flip-chip bonding, solder, etc., are sealed with an epoxy resin composition. Examples of such modules include boards, hybrid ICs, and multi-chip modules; BGAs (Ball Grid Arrays), CSPs (Chip Size Packages), and MCPs (Multi Chip Packages) which have a structure in which elements are mounted on the surface of a support member having terminals for connecting to a printed circuit board formed on its back surface, the elements are connected to the wiring formed on the support member by bumps or wire bonding, and then the elements are sealed with an epoxy resin composition. Furthermore, epoxy resin compositions can also be suitably used in printed circuit boards.

[0207] Methods for encapsulating electronic components using epoxy resin compositions include low-pressure transfer molding, injection molding, and compression molding.

[0208] ≪Manufacturing Method for Electronic Component Devices≫ A method for manufacturing an electronic component device according to one aspect of the present disclosure includes encapsulating an element with an epoxy resin composition selected from the first to fourth embodiments described above. The method for encapsulating the element is not particularly limited and includes the molding method described above. [Examples]

[0209] The embodiments of this disclosure will be described in detail below with reference to examples, but the embodiments of this disclosure are not limited to these examples.

[0210] <<Examples of the First and Second Embodiments>> [Preparation of epoxy resin composition] The following materials were mixed according to the composition shown in Table 1, and the epoxy resin compositions of the examples and comparative examples were prepared using a twin-screw kneader at a mixing temperature of 100°C. Note that the units for the amounts of components in Table 1 are parts by mass, and "-" indicates that the component was not included.

[0211] (Epoxy resin) • Epoxy resin 1: Biphenylene aralkyl type epoxy resin (product name: NC-3000, Nippon Kayaku Co., Ltd., epoxy equivalent 282 g / eq, softening point 56°C) • Epoxy resin 2: Biphenyl-type epoxy resin (Product name: YX-4000, Mitsubishi Chemical Corporation, epoxy equivalent weight 180-192 g / eq, melting point 105°C)

[0212] (Hardening agent) • Hardener: Xylylene-type phenolic resin (product name: MEHC-7800SS, Meiwa Chemicals Co., Ltd., hydroxyl group equivalent 175g / eq, softening point 70℃)

[0213] (Inorganic filler) • Inorganic filler: Spherical silica with an average particle size of 15 μm

[0214] (Additives) • Curing accelerator: Phosphorus-based curing accelerator • Coupling agent: N-phenyl-3-aminopropyltrimethoxysilane (product name: KBM-573, Shin-Etsu Chemical Co., Ltd.) • Release agent: Licowax E (Clariant Chemicals Co., Ltd.) • Coloring agent: Carbon black ·Ion exchanger: Hydrotalcite compound (trade name: DHT-4A, Kyowa Chemical Industry Co., Ltd.) ·Triazine derivative (trade name: VD-5, Shikoku Chemicals Corporation, the following compound, R is a divalent linking group)

[0215] [Chemical formula]

[0216] [Evaluation] The properties of the epoxy resin compositions prepared in the examples and comparative examples were evaluated by the following property tests. Unless otherwise specified, the epoxy resin compositions were molded by a transfer molding machine under the conditions of a mold temperature of 180°C, a molding pressure of 6.9 MPa, and a curing time of 90 seconds. Further, post-curing was carried out at 175°C for 5 hours as necessary.

[0217] (Moisture absorption curing property) The powdery epoxy resin composition was placed in a thermo-hygrostat at 25°C and 50% relative humidity and stored for 24 hours, 48 hours, or 74 hours. After each period of time elapsed, each epoxy resin composition was taken out of the thermo-hygrostat and molded into a disc shape with a diameter of 50 mm and a thickness of 3 mm by a transfer molding machine to prepare test pieces. The hot hardness of each test piece was measured using a Shore D type hardness tester (Ueshima Seisakusho Co., Ltd., HD-1120 (type D)), and the ratio of the hot hardness of each test piece to the hot hardness of the cured product of the epoxy resin composition not stored in the thermo-hygrostat was examined when the hot hardness of the cured product was taken as 100%.

[0218] (Water absorption of cured product) The disc-shaped test pieces molded as described above were post-cured. Thereafter, the obtained test pieces were left standing at 121°C and 2 atm for 20 hours, and the mass change before and after standing was measured. The water absorption was calculated from the measurement results by the following formula. Water absorption (mass %) = (disc mass after standing - disc mass before standing) / disc mass before standing × 100

[0219] (Adhesion) ·Adhesive force to copper (Cu) The epoxy resin composition was molded onto a copper plate under the above conditions to a size of 4 mm in base diameter, 3 mm in top diameter, and 4 mm in height, and then cured under the above conditions. Subsequently, the shear bond strength (MPa) was determined at room temperature or while maintaining the copper plate temperature at 260°C at a shear rate of 50 μm / s using a bond tester (Nordson Advanced Technologies, Inc., Series 4000). Adhesion to silver (Ag) The same test was conducted using silver-plated copper plates instead of copper plates.

[0220] [Table 1]

[0221] Of the components listed in Table 1, all components except the inorganic filler and ion exchanger correspond to tetrahydrofuran-soluble solids. The total mass of epoxy resin and phenol curing agent relative to the total mass of tetrahydrofuran-soluble solids was 92%, 92%, 92%, 91%, and 90% in Comparative Example 1-1, Example 1-1, Example 1-2, Example 1-3, and Example 1-4, respectively.

[0222] As can be seen from Table 1, the epoxy resin compositions of Examples 1-1 to 1-4 exhibit excellent moisture-absorbing and curing properties. Furthermore, the epoxy resin compositions of Examples 1-1 to 1-4 also exhibit excellent adhesion to copper and silver. In addition, although not shown in the table above, it was found that the epoxy resin compositions of Examples 1-1 to 1-4 had lower electrical conductivity in their extracts compared to Comparative Example 1-1. Based on these test results, it is considered that highly reliable electronic component devices can be manufactured using the epoxy resin compositions of Examples 1-1 to 1-4.

[0223] <<Examples of the Third and Fourth Embodiments>> [Preparation of epoxy resin composition] The following materials were mixed according to the compositions shown in Table 2, and the epoxy resin compositions of the examples and comparative examples were prepared using a twin-screw kneader at a mixing temperature of 100°C. Note that the units for the amounts of components in Table 2 are parts by mass, and "-" indicates that the component was not included.

[0224] (Epoxy resin) • Epoxy resin 1: Biphenylene aralkyl type epoxy resin (product name: NC-3000, Nippon Kayaku Co., Ltd., epoxy equivalent 282 g / eq, softening point 56°C) • Epoxy resin 2: Biphenyl-type epoxy resin (Product name: YX-4000, Mitsubishi Chemical Corporation, epoxy equivalent weight 180-192 g / eq, melting point 105°C)

[0225] (Hardening agent) • Hardener: Xylylene-type phenolic resin (product name: MEHC-7800SS, Meiwa Chemicals Co., Ltd., hydroxyl group equivalent 175g / eq, softening point 70℃)

[0226] (Inorganic filler) • Inorganic filler: Spherical silica with an average particle size of 15 μm

[0227] (Additives) • Curing accelerator: Phosphorus-based curing accelerator • Coupling agent: N-phenyl-3-aminopropyltrimethoxysilane (product name: KBM-573, Shin-Etsu Chemical Co., Ltd.) • Release agent: Licowax E (Clariant Chemicals Co., Ltd.) • Coloring agent: Carbon black • Ion exchanger: Hydrotalcite compound (product name: DHT-4A, Kyowa Chemical Industry Co., Ltd., average particle size 0.45 μm) • Triazine derivative (Trade name: VD-5, Shikoku Chemicals Co., Ltd., see compound below, R is a divalent linking group)

[0228] [ka]

[0229] 〔evaluation〕 The properties of the epoxy resin compositions prepared in the examples and comparative examples were evaluated by the following property tests. The results are shown in Table 2. Unless otherwise specified, the epoxy resin compositions were molded using a transfer molding machine under the following conditions: mold temperature of 180°C, molding pressure of 6.9 MPa, and curing time of 90 seconds.

[0230] (Electrical conductivity of epoxy resin composition extract) The hardened material molded using the above method was pulverized, and 5g of the pulverized material and 50g of pure water were placed in a dedicated extraction container and treated at 121°C for 20 hours under 2 atmospheres. After treatment, the material was cooled, and the pulverized material and pure water in the extraction container were filtered out. This filtrate was used as the extract water. The electrical conductivity of the extract water was measured using an electrical conductivity meter.

[0231] (Measurement of ion concentration in epoxy resin composition extract) The ion concentration of the extracted water was measured using an ion chromatograph.

[0232] [Table 2]

[0233] Of the components listed in Table 2, all components except the inorganic filler and ion exchanger correspond to tetrahydrofuran-soluble solids. The total mass of epoxy resin and phenol curing agent relative to the total mass of tetrahydrofuran-soluble solids was 92%, 92%, 92%, 91%, and 90% in Comparative Example 2-1, Example 2-1, Example 2-2, Example 2-3, and Example 2-4, respectively.

[0234] As can be seen from Table 2, the electrical conductivity of the epoxy resin composition extract was remarkably low in Examples 2-1 to 2-4, and the evaluation of moisture resistance reliability was excellent.

[0235] The disclosures of Japanese Patent Applications No. 2020-080703 and No. 2020-080704 are incorporated herein by reference in their entirety. All documents, patent applications, and technical standards described herein are incorporated by reference to the same extent as if each individual document, patent application, and technical standard were specifically and individually noted to be incorporated by reference.

[0236] (Note) The first and second embodiments of this disclosure include the following aspects: <1> An epoxy resin composition for sealing, comprising an epoxy resin, a phenol curing agent, an inorganic filler, and a triazine ring-containing compound, wherein the content of the phenol curing agent is 40 to 250 parts by mass per 100 parts by mass of the epoxy resin. <2> An epoxy resin composition for sealing, comprising an epoxy resin, a phenol curing agent, an inorganic filler, and a triazine ring-containing compound, wherein the total mass of the epoxy resin and the phenol curing agent is 85% by mass or more of the total mass of tetrahydrofuran-soluble solids in the epoxy resin composition for sealing. <3> The ratio of the number of hydroxyl groups in the phenol curing agent to the number of epoxy groups in the epoxy resin in the encapsulating epoxy resin composition (number of hydroxyl groups in the phenol curing agent / number of epoxy groups in the epoxy resin) is 0.8 to 1.2. <1> or <2> The epoxy resin composition for sealing described above. <4> The epoxy resin comprises at least one selected from the group consisting of aralkyl epoxy resins and biphenyl epoxy resins. <1> ~ <3> An epoxy resin composition for sealing according to any one of the items. <5> The triazine ring of the triazine ring-containing compound has a substituent, and the substituent includes a primary amino group. <1> ~ <4> An epoxy resin composition for sealing according to any one of the items. <6> The triazine ring-containing compound includes a compound represented by the following formula (I), where Y represents a monovalent organic group having 1 to 30 carbon atoms and a hydroxyl group, or a monovalent organic group having 1 to 30 carbon atoms and an alkoxysilyl group. <1> ~ <5> An epoxy resin composition for sealing according to any one of the items.

[0237] [ka]

[0238] <7> The content of the triazine ring-containing compound is 0.3 parts by mass to 20 parts by mass per 100 parts by mass of the epoxy resin. <1> ~ <6> An epoxy resin composition for sealing according to any one of the items. <8> Furthermore, the epoxy resin composition for sealing contains 2.0% by mass or more of a silane coupling agent relative to the total mass of the resin components. <1> ~ <7> An epoxy resin composition for sealing according to any one of the items. <9> An element and a seal for the element. <1> ~ <8> An electronic component device comprising a cured product of an epoxy resin composition for sealing as described in any one of the items. <10> <1> ~ <8> A method for manufacturing an electronic component device, comprising sealing an element with an epoxy resin composition for sealing as described in any one of the items.

[0239] The third and fourth embodiments of this disclosure include the following aspects: <1> An epoxy resin composition for sealing, comprising an epoxy resin, a phenol curing agent, an inorganic filler, a triazine ring-containing compound, and a hydrotalcite compound, wherein the content of the phenol curing agent is 40 to 250 parts by mass per 100 parts by mass of the epoxy resin. <2> An epoxy resin composition for sealing, comprising an epoxy resin, a phenol curing agent, an inorganic filler, a triazine ring-containing compound, and a hydrotalcite compound, wherein the total mass of the epoxy resin and the phenol curing agent is 85% by mass or more of the total mass of tetrahydrofuran-soluble solids in the epoxy resin composition for sealing. <3> The ratio of the number of hydroxyl groups in the phenol curing agent to the number of epoxy groups in the epoxy resin in the encapsulating epoxy resin composition (number of hydroxyl groups in the phenol curing agent / number of epoxy groups in the epoxy resin) is 0.8 to 1.2. <1> or <2> The epoxy resin composition for sealing described above. <4> The epoxy resin comprises at least one selected from the group consisting of aralkyl epoxy resins and biphenyl epoxy resins. <1> ~ <3> An epoxy resin composition for sealing according to any one of the items. <5> The triazine ring of the triazine ring-containing compound has a substituent, and the substituent includes a primary amino group. <1> ~ <4> An epoxy resin composition for sealing according to any one of the items. <6> The triazine ring-containing compound includes a compound represented by the following formula (I), where Y represents a monovalent organic group having 1 to 30 carbon atoms and a hydroxyl group, or a monovalent organic group having 1 to 30 carbon atoms and an alkoxysilyl group. <1> ~ <5> An epoxy resin composition for sealing according to any one of the items.

[0240] [ka]

[0241] <7> The content of the triazine ring-containing compound is 0.3 parts by mass to 20 parts by mass per 100 parts by mass of the epoxy resin. <1> ~ <6> An epoxy resin composition for sealing according to any one of the items. <8> An element and a seal for the element. <1> ~ <7> An electronic component device comprising a cured product of an epoxy resin composition for sealing as described in any one of the items. <9> <1> ~ <7> A method for manufacturing an electronic component device, comprising sealing an element with an epoxy resin composition for sealing as described in any one of the items.

Claims

1. It contains epoxy resin, phenol curing agent, inorganic filler, triazine ring-containing compound, and hydrotalcite compound. The content of the phenol curing agent is 40 to 250 parts by mass per 100 parts by mass of the epoxy resin. The triazine ring-containing compound is a compound represented by the following formula (II), where R independently represents a hydrogen atom, a hydroxyl group, a C1-C5 alkyl group, or a C1-C5 alkoxy group, and at least one of the three Rs is an alkoxy group; X is a hydrocarbon group having or not having a nitrogen atom or an oxygen atom, and the number of atoms on the atomic chain between the silicon atom and the carbon atom of the triazine ring in formula (II) is 2 to 13. 【Chemistry 1】 The content of the triazine ring-containing compound is 1.0 to 6.0 parts by mass per 100.0 parts by mass of epoxy resin. Epoxy resin composition for sealing.

2. It contains epoxy resin, phenol curing agent, inorganic filler, triazine ring-containing compound, and hydrotalcite compound. The total mass of the epoxy resin and the phenol curing agent is 85% by mass or more, relative to the total mass of tetrahydrofuran-soluble solids in the epoxy resin composition for sealing. The triazine ring-containing compound is a compound represented by the following formula (II), where R independently represents a hydrogen atom, a hydroxyl group, a C1-C5 alkyl group, or a C1-C5 alkoxy group, and at least one of the three Rs is an alkoxy group; X is a hydrocarbon group having or not having a nitrogen atom or an oxygen atom, and the number of atoms on the atomic chain between the silicon atom and the carbon atom of the triazine ring in formula (II) is 2 to 13. 【Chemistry 2】 The content of the triazine ring-containing compound is 1.0 to 6.0 parts by mass per 100.0 parts by mass of epoxy resin. Epoxy resin composition for sealing.

3. The encapsulating epoxy resin composition according to claim 1 or claim 2, wherein the ratio of the number of hydroxyl groups in the phenol curing agent to the number of epoxy groups in the epoxy resin (number of hydroxyl groups in the phenol curing agent / number of epoxy groups in the epoxy resin) in the encapsulating epoxy resin composition is 0.8 to 1.

2.

4. The epoxy resin composition for sealing according to any one of claims 1 to 3, wherein the epoxy resin comprises at least one selected from the group consisting of aralkyl-type epoxy resins and biphenyl-type epoxy resins.

5. Furthermore, the epoxy resin composition for sealing according to any one of claims 1 to 4 contains 2.0% by mass or more of a silane coupling agent based on the total mass of the epoxy resin and the phenol curing agent.

6. Element and, A cured product of the sealing epoxy resin composition according to any one of claims 1 to 5 for sealing the element, An electronic component device equipped with the following features.

7. A method for manufacturing an electronic component device, comprising sealing an element with the epoxy resin composition for sealing according to any one of claims 1 to 5.

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