JP7298466B2 - resin composition - Google Patents

Description

The present invention relates to resin compositions containing inorganic fillers. Furthermore, the present invention relates to a cured product, a resin sheet, a circuit board, a semiconductor chip package, and a semiconductor device obtained using the resin composition.

In recent years, the demand for compact, high-performance electronic devices such as smartphones and tablet devices has increased, and along with this, there is a demand for even higher functionality in sealing materials for semiconductor chip packages used in these small electronic devices. ing. As such a sealing material, one formed by curing a resin composition is known (Patent Document 1).

In particular, in recent years, there has been a demand for thinner insulating layers or sealing layers used in semiconductor chip packages. However, when the insulating layer or the sealing layer is made thin, warping tends to occur easily. As a method for suppressing warpage, a method of adding an epoxy-modified siloxane or the like capable of relieving stress to a resin composition is known (Patent Document 2).

JP 2017-008312 A JP 2018-172599 A

However, when epoxy-modified siloxane or the like is added to the resin composition, the adhesiveness to the thermal peeling tape used in the semiconductor chip package manufacturing process may decrease, and flow marks are likely to occur after molding. There is Therefore, there is a demand for a resin composition that can suppress warpage, suppress the occurrence of flow marks after molding, and can provide a cured product having excellent adhesion to a thermal release tape. It is

Accordingly, an object of the present invention is to provide a resin composition that can suppress the occurrence of flow marks and warpage after molding, and that can provide a cured product having excellent adhesiveness to a thermal release tape.

In order to achieve the object of the present invention, the present inventors have made intensive studies, and as a result, by using a resin composition containing (A-1) a hydroxyl group-containing siloxane compound and (B) an inorganic filler in a predetermined ratio, mold The inventors have found that it is possible to suppress the occurrence of flow marks and warpage after molding, and to obtain a cured product having excellent adhesiveness to a thermal release tape, thereby completing the present invention.

That is, the present invention includes the following contents.
[1] A resin composition containing (A) a curing agent and (B) an inorganic filler,
(A) component contains (A-1) a hydroxyl group-containing siloxane compound,
The content of the component (A-1) is 0.5% by mass or more and less than 5% by mass when the non-volatile components other than the component (B) in the resin composition are 100% by mass,
A resin composition in which the content of component (B) is 60% by mass or more when all non-volatile components in the resin composition are taken as 100% by mass.
[2] The resin composition according to [1] above, wherein the component (A-1) is a phenolic hydroxyl group-containing siloxane compound.
[3] The resin composition according to [1] or [2] above, wherein component (A-1) has a chain siloxane skeleton.
[4] The resin composition according to any one of [1] to [3] above, wherein the hydroxyl value of component (A-1) is 120 mgKOH/g or less.
[5] The above [1], wherein the component (A) further contains a curing agent selected from a phenol-based curing agent, a naphthol-based curing agent, an amine-based curing agent, an active ester-based curing agent, and an acid anhydride-based curing agent. The resin composition according to any one of -[4].
[6] Any one of [1] to [5] above, wherein the content of component (A-1) is 3% by mass to 20% by mass when all of component (A) is 100% by mass. of the resin composition.
[7] The resin composition according to any one of [1] to [6] above, wherein the component (B) is silica.
[8] The content of component (B) is 70% by mass or more when all non-volatile components in the resin composition are 100% by mass. Resin composition.
[9] The resin composition according to [8] above, wherein the content of component (B) is 80% by mass or more when all non-volatile components in the resin composition are taken as 100% by mass.
[10] The above [1] to [9], wherein the content mass ratio of component (B) to component (A-1) ((B) component/(A-1) component) is 50 to 1,000. The resin composition according to any one of the above.
[11] The resin composition according to any one of [1] to [10] above, further comprising (C) an epoxy resin.
[12] The resin composition according to any one of [1] to [11] above for forming an insulating layer of a semiconductor chip package.
[13] The resin composition according to any one of [1] to [11] above for forming an insulating layer of a circuit board.
[14] The resin composition according to any one of the above [1] to [11] for encapsulating a semiconductor chip in a semiconductor chip package.
[15] A cured product obtained from the resin composition according to any one of [1] to [14] above.
[16] A resin sheet comprising a support and a resin composition layer containing the resin composition according to any one of [1] to [14] provided on the support.
[17] A circuit board comprising an insulating layer formed of a cured product obtained from the resin composition according to any one of [1] to [14] above.
[18] A semiconductor chip package including the circuit board according to [17] above and a semiconductor chip mounted on the circuit board.
[19] A semiconductor chip package comprising a semiconductor chip and a cured product obtained from the resin composition according to any one of [1] to [14] for encapsulating the semiconductor chip.
[20] A semiconductor device comprising the semiconductor chip package according to [18] or [19] above.

INDUSTRIAL APPLICABILITY According to the resin composition of the present invention, it is possible to obtain a cured product that can suppress the occurrence of flow marks and warpage after molding and has excellent adhesion to a thermal release tape.

BEST MODE FOR CARRYING OUT THE INVENTION The present invention will now be described in detail with reference to its preferred embodiments. However, the present invention is not limited to the following embodiments and examples, and can be arbitrarily modified without departing from the scope of the claims of the present invention and their equivalents.

<Resin composition>
The resin composition of the present invention contains (A) a curing agent, and (B) an inorganic filler, and (A) component contains (A-1) a hydroxyl group-containing siloxane compound, and contains component (A-1). The amount is 0.5% by mass or more and less than 5% by mass when the non-volatile components other than the component (B) in the resin composition are 100% by mass, and the content of the component (B) is in the resin composition When all the non-volatile components are 100% by mass, it is 60% by mass or more. By using such a resin composition, generation of flow marks and warpage after molding can be suppressed, and a cured product having excellent adhesiveness to a thermal release tape can be obtained.

In addition to (A) a curing agent and (B) an inorganic filler, the resin composition of the present invention further includes (C) an epoxy resin, (D) a curing accelerator, (E) other additives, and ( F) It may contain an organic solvent. Each component contained in the resin composition will be described in detail below.

<(A) Curing agent>
The resin composition of the present invention contains (A) a curing agent. (A) The curing agent has a function of curing the (C) epoxy resin. (A) The (C) epoxy resin to be cured by the curing agent may be contained in the resin composition of the present invention, or may be separately mixed with the resin composition of the present invention before curing.

The content of (A) the curing agent in the resin composition is not particularly limited. % or less, 95 mass% or less, 85 mass% or less, preferably 75 mass% or less, 70 mass% or less, more preferably 60 mass% or less, 55 mass% or less, further preferably 50 mass% or less, 45 mass% or less , Particularly preferably, it is 42% by mass or less and 40% by mass or less. The lower limit of the content of (A) the curing agent in the resin composition is not particularly limited, but when non-volatile components other than the (B) inorganic filler in the resin composition are 100% by mass, it is preferable is 0.5% by mass or more, 1% by mass or more, 5% by mass or more, 10% by mass or more, more preferably 15% by mass or more, 20% by mass or more, further preferably 25% by mass or more, 30% by mass or more, especially It is preferably 35% by mass or more and 37% by mass or more.

<(A-1) hydroxyl group-containing siloxane compound>
(A) The curing agent contains (A-1) a hydroxyl group-containing siloxane compound. (A-1) The hydroxyl group-containing siloxane compound has one or more (preferably two or more) hydroxyl groups and one or more (preferably two or more, particularly preferably two or more are repeatedly consecutive) A compound having a siloxane (Si—O—Si) bond.

(A-1) The hydroxyl group-containing siloxane compound may be a siloxane compound having a cyclic siloxane skeleton or a siloxane compound having a chain siloxane skeleton. preferable.

(A-1) The number of hydroxyl groups in the hydroxyl group-containing siloxane compound is not particularly limited, but may be preferably 10 or less, more preferably 5 or less per molecule. (A-1) When the hydroxyl group-containing siloxane compound is a hydroxyl group-containing linear siloxane compound, a side chain type having a hydroxyl group in the side chain, a both end type having a hydroxyl group at both ends, and a hydroxyl group at both the side chain and the end may be any of the side chain terminal types having

(A-1) The number of silicon atoms forming a siloxane bond in the hydroxyl group-containing siloxane compound is not particularly limited, but the lower limit in one molecule is preferably 2 or more, more preferably 3 or more, and particularly preferably 5. number or more, and the upper limit is preferably 2,000 or less, more preferably 1,000 or less, and particularly preferably 500 or less.

(A-1) The silicon atom in the hydroxyl group-containing siloxane compound is preferably substituted with a monovalent organic group having or not having a hydroxyl group at all substitutable sites that do not participate in siloxane bond formation. It is more preferably substituted with an optionally substituted monovalent hydrocarbon group with or without

(A-1) The hydroxyl group-containing siloxane compound preferably has the formula (1):

[In the formula, at least two of 2n+2 R ¹ and two R ² independently represent an optionally substituted monovalent hydrocarbon group having one or more hydroxyl groups, and the others independently represents an optionally substituted monovalent hydrocarbon group; or at least two of the 2n+2 R ¹ independently represent an optionally substituted monovalent hydrocarbon group having one or more hydroxyl groups and others independently represent an optionally substituted monovalent hydrocarbon group, and two R ² together represent one —O— and bond to each other to form a cyclic siloxane skeleton. Form. n represents an integer of 2 or more. ]
is a siloxane compound represented by

The "monovalent hydrocarbon group" can be, for example, an alkyl group, an alkenyl group, an aryl group, or a combination thereof, and the combination includes an aryl group, an alkenyl group, and/or an alkyl-substituted aryl group; A group-substituted alkyl group; an aryl group-substituted alkenyl group and the like are included, but are not particularly limited.

"Optionally substituted monovalent hydrocarbon group having one or more hydroxyl groups" means a monovalent hydrocarbon group optionally having one or more substituents, wherein at least one It means a group having a hydroxyl group. “Optionally substituted monovalent hydrocarbon group” means a monovalent hydrocarbon group optionally having one or more substituents (provided that “optional It means having no hydroxyl group, in distinction from "substituted monovalent hydrocarbon group".).

"Alkyl (group)" refers to a linear, branched and/or cyclic monovalent aliphatic saturated hydrocarbon group. "Alkyl (group)" is preferably an alkyl group having 1 to 10 carbon atoms, more preferably an alkyl group having 1 to 6 carbon atoms. Examples of "alkyl (group)" include methyl group, ethyl group, propyl group, isopropyl group, butyl group, isobutyl group, sec-butyl group, tert-butyl group, pentyl group, isopentyl group, neopentyl group, sec- pentyl group, tert-pentyl group, cyclopentyl group, cyclohexyl group, cyclopentylmethyl group and the like.

"Alkenyl (group)" refers to linear, branched and/or cyclic monovalent unsaturated aliphatic hydrocarbon groups having at least one carbon-carbon double bond. "Alkenyl (group)" is preferably an alkenyl group having 2 to 10 carbon atoms, more preferably an alkenyl group having 2 to 6 carbon atoms. Examples of "alkenyl (group)" include, for example, vinyl group, 1-propenyl group, 2-propenyl group, 2-methyl-1-propenyl group, 1-butenyl group, 2-butenyl group, 3-butenyl group, 3- methyl-2-butenyl group, 1-pentenyl group, 2-pentenyl group, 3-pentenyl group, 4-pentenyl group, 4-methyl-3-pentenyl group, 1-hexenyl group, 3-hexenyl group, 5-hexenyl group , 2-cyclohexenyl group and the like.

"Aryl (group)" refers to a monovalent aromatic hydrocarbon group. "Aryl (group)" is preferably an aryl group having 6 to 10 carbon atoms. "Aryl (group)" includes, for example, phenyl group, 1-naphthyl group, 2-naphthyl group and the like.

The optional substituents in the "optionally substituted monovalent hydrocarbon group" are not particularly limited, but examples include halogen atoms, cyano groups, nitro groups, alkyl-oxy groups, mono- or di(alkyl) -amino group, alkyl-carbonyl group, alkyl-oxy-carbonyl group, mono or di(alkyl)-amino-carbonyl group, alkyl-carbonyl-oxy group, mono or di(alkyl-carbonyl)-amino group, alkenyl-oxy group, mono or di(alkenyl)-amino group, alkenyl-carbonyl group, alkenyl-oxy-carbonyl group, mono or di(alkenyl)-amino-carbonyl group, alkenyl-carbonyl-oxy group, mono or di(alkenyl-carbonyl )-amino group, aryl-oxy group, mono- or di(aryl)-amino group, aryl-carbonyl group, aryl-oxy-carbonyl group, mono- or di(aryl)-amino-carbonyl group, aryl-carbonyl-oxy group , mono- or di(aryl-carbonyl)-amino groups, aryl-oxy groups, aryl-carbonyl groups, aryl-oxy-carbonyl groups, aryl-carbonyl-oxy groups, etc., or combinations thereof. The number of substituents is preferably 1 to 3.

In formula (1), the "optionally substituted monovalent hydrocarbon group having one or more hydroxyl groups" is, for example, an alkyl group having one or more hydroxyl groups, an alkenyl group having one or more hydroxyl groups, one an aryl group having a hydroxyl group, an aryl group-substituted alkyl group having one or more hydroxyl groups, an aryl group-substituted alkenyl group having one or more hydroxyl groups, an alkyl group-substituted aryl group having one or more hydroxyl groups, Alkenyl group-substituted aryl groups having one or more hydroxyl groups, aryl group-substituted aryl groups having one or more hydroxyl groups, and the like, alkyl groups having one or more hydroxyl groups, or having one or more hydroxyl groups It is preferably an aryl group-substituted alkyl group. The number of hydroxyl groups in the "optionally substituted monovalent hydrocarbon group having one or more hydroxyl groups" is preferably 1 to 3, particularly preferably 1. "Optionally substituted monovalent hydrocarbon groups having one or more hydroxyl groups" are preferably bonded to different silicon atoms. In one embodiment, the hydroxyl group is preferably a phenolic hydroxyl group by virtue of being on an aryl (group). That is, in one embodiment, (A-1) the hydroxyl group-containing siloxane compound is preferably a phenolic hydroxyl group-containing siloxane compound (C) from the viewpoint of reactivity with the epoxy resin.

In formula (1), the "optionally substituted monovalent hydrocarbon group" is, for example, an alkyl group, an alkenyl group, an aryl group, an aryl group-substituted alkyl group, an aryl group-substituted alkenyl group, or an alkyl group-substituted aryl group. , an alkenyl group-substituted aryl group, an aryl group-substituted aryl group, etc., preferably an alkyl group, particularly preferably a methyl group.

In formula (1), preferably at least two of 2n+2 R ¹ and two R ² are independently optionally substituted monovalent hydrocarbon groups having one or more hydroxyl groups, and others are independently optionally substituted monovalent hydrocarbon groups that do not form a cyclic siloxane skeleton and are chain siloxanes. More preferably, at least two of 2n+2 R ¹ and two R ² are independently monovalent hydrocarbon groups having one or more hydroxyl groups, and the others are independently It is a monovalent hydrocarbon group. More preferably, at least two of 2n+2 R ¹ and two R ² are independently alkyl groups having one or more hydroxyl groups, or aryl group-substituted alkyl groups having one or more hydroxyl groups and the others are independently alkyl groups.

In formula (1), n represents an integer of 1 or more, preferably an integer of 2 to 2,000, more preferably an integer of 2 to 1,000, still more preferably an integer of 5 to 500 be.

(A-1) Commercial products of hydroxyl group-containing siloxane compounds include, for example, Shin-Etsu Chemical Co., Ltd. "X-22-160AS", "KF-6001", "KF-6002", "KF-6003", "X -22-4039", "X-22-4015" (carbinol-type hydroxyl group-containing siloxane compound), Shin-Etsu Chemical Co., Ltd. "KF-2201", "X-22-1821" (phenolic hydroxyl group-containing siloxane compound), etc. is mentioned.

(A-1) The weight average molecular weight (Mw) of the hydroxyl group-containing siloxane compound is preferably 50,000 or less, more preferably 20,000 or less. The lower limit of the weight average molecular weight (Mw) can be preferably 500 or more, more preferably 1,000 or more. (A-1) The number average molecular weight (Mn) of the hydroxyl group-containing siloxane compound is preferably 50,000 or less, more preferably 20,000 or less. The lower limit of the number average molecular weight (Mn) can be preferably 500 or more, more preferably 1,000 or more. The weight average molecular weight (Mw) and number average molecular weight (Mn) can be measured by a gel permeation chromatography (GPC) method (converted to polystyrene).

(A-1) The hydroxyl value of the hydroxyl-containing siloxane compound is preferably 200 mgKOH/g or less, more preferably 150 mgKOH/g or less, even more preferably 120 mgKOH/g or less, even more preferably 100 mgKOH/g or less, and particularly preferably 80 mgKOH. /g or less. The lower limit of hydroxyl value is preferably 10 mgKOH/g or more, more preferably 15 mgKOH/g or more, still more preferably 20 mgKOH/g or more, still more preferably 25 mgKOH/g or more, and particularly preferably 30 mgKOH/g or more. The hydroxyl value indicates the amount of potassium hydroxide (mg per 1 g of the compound) required to neutralize the free acetic acid when the hydroxyl group of the compound is acetylated with acetic anhydride.

(A-1) The hydroxyl group equivalent of the hydroxyl group-containing siloxane compound is preferably 10,000 g/eq. Below, more preferably 5,000 g/eq. Below, more preferably 3,000 g/eq. Below, particularly preferably 2,000 g/eq. can be: The lower limit of hydroxyl equivalent is preferably 100 g/eq. above, more preferably 200 g/eq. above, more preferably 500 g/eq. above, particularly preferably 700 g/eq. It can be more than A hydroxyl equivalent is the mass (g) of a compound per equivalent of hydroxyl.

(A-1) The viscosity (25° C.) of the hydroxyl group-containing siloxane compound is preferably 1,000 mm ² s or less, more preferably 500 mm ² s or less, still more preferably 200 mm ² s or less, and particularly preferably 100 mm ² • may be less than or equal to s; The lower limit of the viscosity (25°C) is preferably 10 mm ² ·s or more, more preferably 30 mm ² ·s or more, still more preferably 50 mm ² ·s or more, and particularly preferably 60 mm ² ·s or more.

The content of the (A-1) hydroxyl group-containing siloxane compound in the resin composition is 0.5% by mass or more when the non-volatile components other than the (B) inorganic filler in the resin composition is 100% by mass. , preferably 1% by mass or more, more preferably 1.5% by mass or more, still more preferably 1.8% by mass or more, and particularly preferably 2% by mass or more. The upper limit of the content of (A-1) a hydroxyl group-containing siloxane compound in the resin composition is less than 5% by mass when the non-volatile components other than the (B) inorganic filler in the resin composition are taken as 100% by mass. , preferably less than 4.5% by weight.

<Optional curing agent other than component (A-1)>
The resin composition of the present invention may further contain any curing agent other than component (A-1).

Any curing agent other than component (A-1) is a curing agent that does not have a hydroxyl group or a siloxane bond, for example, an atom selected from hydrogen, carbon, oxygen, nitrogen, and sulfur atoms. It may be a compound capable of curing the (C) epoxy resin as a constituent atom. Optional curing agents other than the component (A-1) are not particularly limited, but examples include phenolic curing agents, naphthol curing agents, acid anhydride curing agents, amine curing agents, and active esters. curing agents, benzoxazine-based curing agents, cyanate ester-based curing agents, and carbodiimide-based curing agents. Any curing agent other than component (A-1) may be used alone or in combination of two or more. Any curing agent other than component (A-1) contains a curing agent selected from a phenol curing agent, a naphthol curing agent, an amine curing agent, an active ester curing agent, and an acid anhydride curing agent. is preferred, and it is particularly preferred to contain an acid anhydride curing agent.

As the phenolic curing agent and the naphtholic curing agent, a phenolic curing agent having a novolac structure or a naphtholic curing agent having a novolac structure is preferable from the viewpoint of heat resistance and water resistance. From the viewpoint of adhesion to adherends, a nitrogen-containing phenolic curing agent or a nitrogen-containing naphthol curing agent is preferable, and a triazine skeleton-containing phenolic curing agent or a triazine skeleton-containing naphthol curing agent is more preferable. Among them, a triazine skeleton-containing phenol novolak resin is preferable from the viewpoint of highly satisfying heat resistance, water resistance, and adhesion. Specific examples of phenol-based curing agents and naphthol-based curing agents include "MEH-7700", "MEH-7810" and "MEH-7851" manufactured by Meiwa Kasei Co., Ltd., "NHN" manufactured by Nippon Kayaku Co., Ltd., "CBN", "GPH", Nippon Steel Chemical & Materials "SN-170", "SN-180", "SN-190", "SN-475", "SN-485", "SN-495" ”, “SN-375”, “SN-395”, DIC “LA-7052”, “LA-7054”, “LA-3018”, “LA-3018-50P”, “LA-1356”, "TD2090", "TD-2090-60M" and the like.

Acid anhydride curing agents include curing agents having one or more acid anhydride groups in one molecule, and curing agents having two or more acid anhydride groups in one molecule are preferred. Specific examples of acid anhydride curing agents include phthalic anhydride, tetrahydrophthalic anhydride, hexahydrophthalic anhydride, methyltetrahydrophthalic anhydride, methylhexahydrophthalic anhydride, methylnadic anhydride, and hydrogenated methylnadic acid. anhydride, trialkyltetrahydrophthalic anhydride, dodecenylsuccinic anhydride, 5-(2,5-dioxotetrahydro-3-furanyl)-3-methyl-3-cyclohexene-1,2-dicarboxylic anhydride, trianhydride mellitic acid, pyromellitic anhydride, benzophenonetetracarboxylic dianhydride, biphenyltetracarboxylic dianhydride, naphthalenetetracarboxylic dianhydride, oxydiphthalic dianhydride, 3,3'-4,4'- Diphenylsulfonetetracarboxylic dianhydride, 1,3,3a,4,5,9b-hexahydro-5-(tetrahydro-2,5-dioxo-3-furanyl)-naphtho[1,2-C]furan-1 , 3-dione, ethylene glycol bis(anhydrotrimellitate), polymer-type acid anhydrides such as styrene/maleic acid resin obtained by copolymerizing styrene and maleic acid. Commercially available acid anhydride-based curing agents include "HNA-100", "MH-700", "MTA-15", "DDSA" and "OSA" manufactured by Shin Nippon Rika Co., Ltd., and " YH-306”, “YH-307”, “HN-2200” and “HN-5500” manufactured by Hitachi Chemical Co., Ltd., and the like.

Amine-based curing agents include curing agents having one or more, preferably two or more amino groups in one molecule. Examples include aliphatic amines, polyether amines, alicyclic amines, Aromatic amines and the like can be mentioned, and among them, aromatic amines are preferable from the viewpoint of achieving the desired effects of the present invention. Amine-based curing agents are preferably primary amines or secondary amines, more preferably primary amines. Specific examples of amine-based curing agents include 4,4′-methylenebis(2,6-dimethylaniline), diphenyldiaminosulfone, 4,4′-diaminodiphenylmethane, 4,4′-diaminodiphenylsulfone, and 3,3′. -diaminodiphenyl sulfone, m-phenylenediamine, m-xylylenediamine, diethyltoluenediamine, 4,4'-diaminodiphenyl ether, 3,3'-dimethyl-4,4'-diaminobiphenyl, 2,2'-dimethyl- 4,4'-diaminobiphenyl, 3,3'-dihydroxybenzidine, 2,2-bis(3-amino-4-hydroxyphenyl)propane, 3,3-dimethyl-5,5-diethyl-4,4-diphenylmethane Diamine, 2,2-bis(4-aminophenyl)propane, 2,2-bis(4-(4-aminophenoxy)phenyl)propane, 1,3-bis(3-aminophenoxy)benzene, 1,3- bis(4-aminophenoxy)benzene, 1,4-bis(4-aminophenoxy)benzene, 4,4′-bis(4-aminophenoxy)biphenyl, bis(4-(4-aminophenoxy)phenyl)sulfone, bis(4-(3-aminophenoxy)phenyl)sulfone, and the like. Commercially available amine-based curing agents may be used. Kayahard AS", "Epicure W" manufactured by Mitsubishi Chemical Co., Ltd., and the like.

The active ester-based curing agent is not particularly limited, but generally contains an ester group with high reaction activity such as phenol esters, thiophenol esters, N-hydroxyamine esters, esters of heterocyclic hydroxy compounds in one molecule. A compound having two or more is preferably used. The active ester curing agent is preferably obtained by a condensation reaction between a carboxylic acid compound and/or a thiocarboxylic acid compound and a hydroxy compound and/or a thiol compound. In particular, from the viewpoint of improving heat resistance, an active ester curing agent obtained from a carboxylic acid compound and a hydroxy compound is preferred, and an active ester curing agent obtained from a carboxylic acid compound and a phenol compound and/or a naphthol compound is more preferred. Examples of carboxylic acid compounds include benzoic acid, acetic acid, succinic acid, maleic acid, itaconic acid, phthalic acid, isophthalic acid, terephthalic acid, and pyromellitic acid. Examples of phenol compounds or naphthol compounds include hydroquinone, resorcinol, bisphenol A, bisphenol F, bisphenol S, phenolphthalin, methylated bisphenol A, methylated bisphenol F, methylated bisphenol S, phenol, o-cresol, m- cresol, p-cresol, catechol, α-naphthol, β-naphthol, 1,5-dihydroxynaphthalene, 1,6-dihydroxynaphthalene, 2,6-dihydroxynaphthalene, dihydroxybenzophenone, trihydroxybenzophenone, tetrahydroxybenzophenone, phloroglucine, Benzenetriol, dicyclopentadiene-type diphenol compound, phenol novolak, and the like. Here, the term "dicyclopentadiene-type diphenol compound" refers to a diphenol compound obtained by condensing one molecule of dicyclopentadiene with two molecules of phenol.

Specifically, an active ester compound containing a dicyclopentadiene type diphenol structure, an active ester compound containing a naphthalene structure, an active ester compound containing an acetylated product of phenol novolac, and an active ester compound containing a benzoylated product of phenol novolak are preferred. Among them, an active ester compound containing a naphthalene structure and an active ester compound containing a dicyclopentadiene-type diphenol structure are more preferable. "Dicyclopentadiene-type diphenol structure" represents a divalent structural unit consisting of phenylene-dicyclopentalene-phenylene.

Commercially available active ester curing agents include, as active ester compounds containing a dicyclopentadiene type diphenol structure, "EXB9451", "EXB9460", "EXB9460S", "HPC-8000", "HPC-8000H", " HPC-8000-65T", "HPC-8000H-65TM", "EXB-8000L", "EXB-8000L-65M", "EXB-8000L-65TM" (manufactured by DIC); active ester compounds containing a naphthalene structure "EXB-9416-70BK", "EXB-8150-65T", "EXB-8100L-65T", "EXB-8150L-65T" (manufactured by DIC Corporation); "DC808" (manufactured by Mitsubishi Chemical Corporation); "YLH1026" (manufactured by Mitsubishi Chemical Corporation), "YLH1030" (manufactured by Mitsubishi Chemical Corporation) and "YLH1048" (manufactured by Mitsubishi Chemical Corporation) as active ester curing agents that are benzoyl compounds of phenol novolak manufactured by); and the like.

Specific examples of benzoxazine-based curing agents include "JBZ-OP100D" and "ODA-BOZ" manufactured by JFE Chemical Co., Ltd.; "HFB2006M" manufactured by Showa Polymer Co., Ltd.; Examples include "Fa".

Examples of cyanate ester curing agents include bisphenol A dicyanate, polyphenolcyanate (oligo(3-methylene-1,5-phenylenecyanate)), 4,4'-methylenebis(2,6-dimethylphenylcyanate), 4, 4′-ethylidene diphenyl dicyanate, hexafluorobisphenol A dicyanate, 2,2-bis(4-cyanate)phenylpropane, 1,1-bis(4-cyanatophenylmethane), bis(4-cyanate-3,5- Difunctional cyanate resins such as dimethylphenyl)methane, 1,3-bis(4-cyanatophenyl-1-(methylethylidene))benzene, bis(4-cyanatophenyl)thioether, and bis(4-cyanatophenyl)ether, Polyfunctional cyanate resins derived from phenol novolak, cresol novolak, etc., and prepolymers obtained by partially triazine-forming these cyanate resins. Specific examples of cyanate ester curing agents include "PT30" and "PT60" (both phenol novolac type polyfunctional cyanate ester resins), "BA230" and "BA230S75" (part of bisphenol A dicyanate) manufactured by Lonza Japan Co., Ltd. or a prepolymer that is entirely triazined to form a trimer), and the like.

Specific examples of carbodiimide curing agents include "V-03" and "V-07" manufactured by Nisshinbo Chemical Co., Ltd., and the like.

The reactive group equivalent of any curing agent other than component (A-1) is preferably 50 g/eq. ~3,000 g/eq. , more preferably 100 g/eq. ~1,000g/eq. , more preferably 100 g/eq. ~500 g/eq. , particularly preferably 100 g/eq. ~300 g/eq. is. Reactive group equivalent weight is the mass of curing agent per equivalent of reactive group. The reactive group is, for example, an aromatic hydroxyl group in the case of a phenol-based curing agent and a naphthol-based curing agent, an active ester group in the case of an active ester-based curing agent, and an acid anhydride group in the case of an acid anhydride-based curing agent. , depending on the type of hardener.

The content of any curing agent other than component (A-1) in the resin composition is not particularly limited. If, for example, 99.5% by mass or less, 95% by mass or less, 90% by mass or less, 80% by mass or less, preferably 70% by mass or less, 60% by mass or less, more preferably 50% by mass or less, 45% by mass % or less, more preferably 40 mass % or less, 38 mass % or less, and particularly preferably 36 mass % or less. The lower limit of the content of any curing agent other than component (A-1) in the resin composition is not particularly limited. % by mass, for example, 0% by mass or more, 5% by mass or more, 10% by mass or more, 15% by mass or more, 20% by mass or more, 25% by mass or more, 30% by mass or more, 32% by mass or more, 34% by mass % or more.

(A) When the curing agent contains any curing agent other than component (A-1), the content of (A-1) hydroxyl group-containing siloxane compound in the resin composition is not particularly limited, (A) When the total amount of the curing agent is 100% by mass, preferably 0.01% by mass or more, more preferably 0.1% by mass or more, still more preferably 1% by mass or more, and even more preferably 3% by mass or more, Particularly preferably, it is 5% by mass or more. The upper limit of the content of (A-1) the hydroxyl group-containing siloxane compound in the resin composition is not particularly limited, but when the total amount of the curing agent (A) is 100% by mass, it is preferably 80% by mass or less. , more preferably 50% by mass or less, still more preferably 30% by mass or less, even more preferably 20% by mass or less, and particularly preferably 15% by mass or less.

<(B) Inorganic filler>
The resin composition of the present invention further contains (B) an inorganic filler.

(B) The material of the inorganic filler is not particularly limited, but examples include silica, alumina, glass, cordierite, silicon oxide, barium sulfate, barium carbonate, talc, clay, mica powder, zinc oxide, hydrotalcite, Boehmite, aluminum hydroxide, magnesium hydroxide, calcium carbonate, magnesium carbonate, magnesium oxide, boron nitride, aluminum nitride, manganese nitride, aluminum borate, strontium carbonate, strontium titanate, calcium titanate, magnesium titanate, bismuth titanate , titanium oxide, zirconium oxide, barium titanate, barium zirconate titanate, barium zirconate, calcium zirconate, zirconium phosphate, and zirconium tungstate phosphate, with silica and alumina being particularly preferred. Examples of silica include amorphous silica, fused silica, crystalline silica, synthetic silica, and hollow silica. As silica, spherical silica is preferable. (B) The inorganic filler may be used singly or in combination of two or more.

(B) Commercially available inorganic fillers include, for example, “UFP-30” manufactured by Denka Kagaku Kogyo; “SP60-05” and “SP507-05” manufactured by Nippon Steel & Sumikin Materials; "YC100C", "YA050C", "YA050C-MJE", "YA010C"; "UFP-30" manufactured by Denka; 5N”; “SC2500SQ”, “SO-C4”, “SO-C2” and “SO-C1” manufactured by Admatechs; “DAW-03” and “FB-105FD” manufactured by Denka.

The average particle size of the inorganic filler (B) is not particularly limited, but is preferably 40 µm or less, more preferably 30 µm or less, still more preferably 20 µm or less, even more preferably 15 µm or less, and particularly preferably 10 µm or less. is. The lower limit of the average particle size of the inorganic filler is not particularly limited, but is preferably 0.01 μm or more, more preferably 0.05 μm or more, still more preferably 0.5 μm or more, still more preferably 1 μm or more, and It is more preferably 3 µm or more, and particularly preferably 5 µm or more. The average particle size of the inorganic filler can be measured by a laser diffraction/scattering method based on Mie scattering theory. Specifically, the particle size distribution of the inorganic filler is prepared on a volume basis using a laser diffraction/scattering type particle size distribution measuring device, and the median diameter can be used as the average particle size for measurement. A measurement sample can be obtained by weighing 100 mg of an inorganic filler and 10 g of methyl ethyl ketone in a vial and dispersing them with ultrasonic waves for 10 minutes. A measurement sample is measured using a laser diffraction particle size distribution measuring device, the wavelengths of the light source used are blue and red, the volume-based particle size distribution of the inorganic filler is measured by the flow cell method, and from the obtained particle size distribution The average particle diameter was calculated as the median diameter. Examples of the laser diffraction particle size distribution analyzer include "LA-960" manufactured by Horiba, Ltd., and the like.

Although the specific surface area of the inorganic filler (B) is not particularly limited, it is preferably 0.01 m ² /g or more, more preferably 0.1 m ² /g or more, and particularly preferably 0.2 m ² /g. That's it. Although there is no particular upper limit, it is preferably 50 m ² /g or less, more preferably 20 m ² /g or less, 10 m ² /g or less, or 5 m ² /g or less. The specific surface area of the inorganic filler is determined by adsorbing nitrogen gas on the sample surface using a specific surface area measuring device (Macsorb HM-1210 manufactured by Mountech) according to the BET method, and calculating the specific surface area using the BET multipoint method. obtained by

(B) Inorganic fillers include aminosilane-based coupling agents, epoxysilane-based coupling agents, mercaptosilane-based coupling agents, alkoxysilane compounds, organosilazane compounds, titanate-based coupling agents, from the viewpoint of improving moisture resistance and dispersibility. It is preferably treated with one or more surface treatment agents such as agents. Examples of commercially available surface treatment agents include "KBM403" (3-glycidoxypropyltrimethoxysilane) manufactured by Shin-Etsu Chemical Co., Ltd., "KBM803" (3-mercaptopropyltrimethoxysilane) manufactured by Shin-Etsu Chemical Co., Ltd., Shin-Etsu Chemical Industry Co., Ltd. "KBE903" (3-aminopropyltriethoxysilane), Shin-Etsu Chemical Co., Ltd. "KBM573" (N-phenyl-3-aminopropyltrimethoxysilane), Shin-Etsu Chemical Co., Ltd. "SZ-31" ( Hexamethyldisilazane), Shin-Etsu Chemical Co., Ltd. "KBM103" (phenyltrimethoxysilane), Shin-Etsu Chemical Co., Ltd. "KBM-4803" (long-chain epoxy type silane coupling agent), Shin-Etsu Chemical Co., Ltd. "KBM- 7103” (3,3,3-trifluoropropyltrimethoxysilane), “KBM503” (3-methacryloxypropyltrimethoxysilane) manufactured by Shin-Etsu Chemical Co., Ltd., “KBM5783” manufactured by Shin-Etsu Chemical Co., Ltd., and the like.

From the viewpoint of improving the dispersibility of the inorganic filler, the degree of surface treatment with the surface treatment agent is preferably within a predetermined range. Specifically, 100% by mass of the inorganic filler is preferably surface-treated with a surface treatment agent of 0.2% to 5% by mass, and is surface-treated with 0.2% to 3% by mass. more preferably 0.3 mass % to 2 mass % of the surface treatment.

The degree of surface treatment by the surface treatment agent can be evaluated by the amount of carbon per unit surface area of the inorganic filler. The amount of carbon per unit surface area of the inorganic filler is preferably 0.02 mg/m ² or more, more preferably 0.1 mg/m ² or more, and more preferably 0.2 mg/m ² from the viewpoint of improving the dispersibility of the inorganic filler. The above is more preferable. On the other hand, from the viewpoint of preventing an increase in the melt viscosity of the resin composition and the melt viscosity in the form of a sheet, it is preferably 1.0 mg/m ² or less, more preferably 0.8 mg/m ² or less, and 0.5 mg/m ^{2 or less} . More preferred are:

(B) The amount of carbon per unit surface area of the inorganic filler can be measured after the surface-treated inorganic filler is washed with a solvent (eg, methyl ethyl ketone (MEK)). Specifically, a sufficient amount of MEK as a solvent is added to the inorganic filler surface-treated with the surface treatment agent, and ultrasonic cleaning is performed at 25° C. for 5 minutes. After removing the supernatant liquid and drying the solid content, a carbon analyzer can be used to measure the amount of carbon per unit surface area of the inorganic filler. As a carbon analyzer, "EMIA-320V" manufactured by Horiba Ltd. can be used.

The content of the inorganic filler (B) in the resin composition is 60% by mass or more, preferably 65% by mass or more, more preferably 65% by mass or more, when all non-volatile components in the resin composition are 100% by mass. 70% by mass or more and 75% by mass or more, more preferably 78% by mass or more and 80% by mass or more, and particularly preferably 82% by mass or more and 83% by mass or more. The upper limit of the content of the inorganic filler (B) in the resin composition is not particularly limited, but when all non-volatile components in the resin composition are 100% by mass, for example, 98% by mass or less. , 95% by mass or less, 90% by mass or less, and the like.

The content mass ratio of the inorganic filler (B) to the hydroxyl group-containing siloxane compound (A-1) in the resin composition ((B) component/(A-1) component) is not particularly limited, but is preferred. is 20 or more, more preferably 50 or more, still more preferably 80 or more, and particularly preferably 100 or more. The upper limit of the content mass ratio ((B) component/(A-1) component) is not particularly limited, but is preferably 2,000 or less, more preferably 1,000 or less, still more preferably 500 or less, Especially preferably, it is 350 or less.

<(C) Epoxy resin>
The resin composition of the present invention may further contain (C) an epoxy resin as an optional component. (C) Epoxy resin means a resin having an epoxy group. (C) Epoxy resin can be a component that is cured by (A) a curing agent.

(C) Epoxy resins include, for example, bixylenol type epoxy resin, bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol S type epoxy resin, bisphenol AF type epoxy resin, dicyclopentadiene type epoxy resin, and trisphenol type epoxy resin. Epoxy resin, naphthol novolak type epoxy resin, phenol novolac type epoxy resin, tert-butyl-catechol type epoxy resin, naphthalene type epoxy resin, naphthol type epoxy resin, anthracene type epoxy resin, glycidylamine type epoxy resin, glycidyl ester type epoxy resin , glycyrrol type epoxy resin, cresol novolac type epoxy resin, phenol aralkyl type epoxy resin, biphenyl type epoxy resin, linear aliphatic epoxy resin, epoxy resin having a butadiene structure, alicyclic epoxy resin, heterocyclic epoxy resin, spiro Ring-containing epoxy resin, cyclohexane type epoxy resin, cyclohexanedimethanol type epoxy resin, naphthylene ether type epoxy resin, trimethylol type epoxy resin, tetraphenylethane type epoxy resin, isocyanurate type epoxy resin, phenolphthalimidine type epoxy resin resins, phenolphthalein-type epoxy resins, and the like. (C) An epoxy resin may be used individually by 1 type, and may be used in combination of 2 or more types.

The resin composition preferably contains an epoxy resin having two or more epoxy groups in one molecule as (C) the epoxy resin. (C) The ratio of the epoxy resin having two or more epoxy groups in one molecule to 100% by mass of the non-volatile component of the epoxy resin is preferably 50% by mass or more, more preferably 60% by mass or more, and particularly preferably is 70% by mass or more.

Epoxy resins include liquid epoxy resins at a temperature of 20° C. (hereinafter sometimes referred to as “liquid epoxy resins”) and solid epoxy resins at a temperature of 20° C. (hereinafter sometimes referred to as “solid epoxy resins”). ). As the epoxy resin, the resin composition of the present invention may contain only a liquid epoxy resin, may contain only a solid epoxy resin, or may contain a combination of a liquid epoxy resin and a solid epoxy resin. You can stay. The epoxy resin in the resin composition of the present invention is preferably a combination of a liquid epoxy resin and a solid epoxy resin.

A liquid epoxy resin having two or more epoxy groups in one molecule is preferable as the liquid epoxy resin.

Liquid epoxy resins include bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol AF type epoxy resin, naphthalene type epoxy resin, glycidyl ester type epoxy resin, glycidyl amine type epoxy resin, glycyrrol type epoxy resin, phenol novolac type epoxy resin. Resins, alicyclic epoxy resins having an ester skeleton, cyclohexane-type epoxy resins, dicyclopentadiene-type epoxy resins, cyclohexanedimethanol-type epoxy resins, and epoxy resins having a butadiene structure are preferred.

Specific examples of liquid epoxy resins include "HP4032", "HP4032D", and "HP4032SS" (naphthalene type epoxy resins) manufactured by DIC; "828US", "828EL", "jER828EL", and "825" manufactured by Mitsubishi Chemical Corporation; ", "Epikote 828EL" (bisphenol A type epoxy resin); "jER807" and "1750" (bisphenol F type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "jER152" (phenol novolac type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "630", "630LSD", "604" (glycidylamine type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "ED-523T" (glycirrol type epoxy resin) manufactured by ADEKA; "EP-3950L" manufactured by ADEKA; "EP-3980S" (glycidylamine type epoxy resin); "EP-4088S" (dicyclopentadiene type epoxy resin) manufactured by ADEKA; "ZX1059" manufactured by Nippon Steel Chemical & Materials (bisphenol A type epoxy resin and bisphenol F-type epoxy resin mixture); "EX-721" (glycidyl ester type epoxy resin) manufactured by Nagase ChemteX; "Celoxide 2021P" manufactured by Daicel (alicyclic epoxy resin having an ester skeleton); Daicel "PB-3600" manufactured by Nippon Soda Co., Ltd. "JP-100" and "JP-200" (epoxy resins having a butadiene structure); 1,4-glycidylcyclohexane type epoxy resin) and the like. These may be used individually by 1 type, and may be used in combination of 2 or more types.

The solid epoxy resin is preferably a solid epoxy resin having 3 or more epoxy groups per molecule, more preferably an aromatic solid epoxy resin having 3 or more epoxy groups per molecule.

Solid epoxy resins include bixylenol type epoxy resin, naphthalene type epoxy resin, naphthalene type tetrafunctional epoxy resin, naphthol novolak type epoxy resin, cresol novolak type epoxy resin, dicyclopentadiene type epoxy resin, trisphenol type epoxy resin, Naphthol type epoxy resin, biphenyl type epoxy resin, naphthylene ether type epoxy resin, anthracene type epoxy resin, bisphenol A type epoxy resin, bisphenol AF type epoxy resin, phenol aralkyl type epoxy resin, tetraphenylethane type epoxy resin, phenol phthalate A mijin-type epoxy resin and a phenolphthalein-type epoxy resin are preferred.

Specific examples of solid epoxy resins include "HP4032H" (naphthalene-type epoxy resin) manufactured by DIC; "HP-4700" and "HP-4710" (naphthalene-type tetrafunctional epoxy resin) manufactured by DIC; "N-690" (cresol novolac type epoxy resin) manufactured by DIC Corporation; "N-695" (cresol novolak type epoxy resin) manufactured by DIC Corporation; "HP-7200", "HP-7200HH", "HP -7200H", "HP-7200L" (dicyclopentadiene type epoxy resin); DIC's "EXA-7311", "EXA-7311-G3", "EXA-7311-G4", "EXA-7311-G4S" ", "HP6000" (naphthylene ether type epoxy resin); Nippon Kayaku "EPPN-502H" (trisphenol type epoxy resin); Nippon Kayaku "NC7000L" (naphthol novolac type epoxy resin); "NC3000H", "NC3000", "NC3000L", "NC3000FH", "NC3100" (biphenyl type epoxy resin) manufactured by Nippon Kayaku; "ESN475V" (naphthalene type epoxy resin) manufactured by Nippon Steel Chemical &Materials; "ESN485" (naphthol type epoxy resin) manufactured by Nippon Steel Chemical &Materials; "ESN375" (dihydroxynaphthalene type epoxy resin) manufactured by Nippon Steel Chemical &Materials; "YX4000H" and "YX4000" manufactured by Mitsubishi Chemical; "YX4000HK", "YL7890" (bixylenol type epoxy resin); "YL6121" (biphenyl type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "YX8800" (anthracene type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "YX7700" (phenol aralkyl type epoxy resin); "PG-100" and "CG-500" manufactured by Osaka Gas Chemicals; "YL7760" (bisphenol AF type epoxy resin) manufactured by Mitsubishi Chemical; "YL7800" (fluorene type epoxy resin); "jER1010" (bisphenol A type epoxy resin) manufactured by Mitsubishi Chemical; "jER1031S" (tetraphenylethane type epoxy resin) manufactured by Mitsubishi Chemical; WHR991S" (phenolphthalimidine type epoxy resin) and the like. These may be used individually by 1 type, and may be used in combination of 2 or more types.

When a liquid epoxy resin and a solid epoxy resin are used together as the component (C), the mass ratio of the solid epoxy resin to the liquid epoxy resin (solid epoxy resin/liquid epoxy resin) is not particularly limited. is preferably 0.2 or more, more preferably 0.5 or more, still more preferably 1 or more, even more preferably 1.3 or more, and particularly preferably 1.5 or more. The upper limit of the mass ratio of solid epoxy resin to liquid epoxy resin (solid epoxy resin/liquid epoxy resin) is not particularly limited, but is preferably 10 or less, more preferably 5 or less, and still more preferably 3 or less. , still more preferably 2 or less, and particularly preferably 1.8 or less.

(C) The epoxy equivalent of the epoxy resin is preferably 50 g/eq. ~5,000g/eq. , more preferably 60 g/eq. ~2,000 g/eq. , more preferably 70 g/eq. ~1,000 g/eq. , even more preferably 80 g/eq. ~500 g/eq. is. Epoxy equivalent weight is the mass of resin per equivalent of epoxy groups. This epoxy equivalent can be measured according to JIS K7236.

(C) The weight average molecular weight (Mw) of the epoxy resin is preferably 100 to 5,000, more preferably 250 to 3,000, still more preferably 400 to 1,500. The weight average molecular weight of the resin can be measured as a polystyrene-equivalent value by a gel permeation chromatography (GPC) method.

When the resin composition of the present invention contains (C) epoxy resin, the amount ratio of (C) epoxy resin and (A) curing agent is [number of epoxy groups of (C) epoxy resin]:[(A) curing agent The ratio of the number of reactive groups ((A-1) the number of hydroxyl groups of the hydroxyl group-containing siloxane compound and the number of reactive groups of the curing agent other than (A-1))] is 1:0.2 to 1:2 is preferred, 1:0.3 to 1:1.5 is more preferred, and 1:0.4 to 1:1.4 is even more preferred.

The content of the (C) epoxy resin in the resin composition is not particularly limited, but is preferably 90% when the non-volatile components other than the (B) inorganic filler in the resin composition are 100% by mass. 85% by mass or less, more preferably 80% by mass or less and 75% by mass or less, still more preferably 70% by mass or less and 67% by mass or less, and particularly preferably 65% by mass or less and 63% by mass or less. The lower limit of the content of the (C) epoxy resin in the resin composition is not particularly limited, but when the non-volatile components other than the (B) inorganic filler in the resin composition are 100% by mass, for example 0% by mass or more, 10% by mass or more, 20% by mass or more, 30% by mass or more, preferably 40% by mass or more, more preferably 50% by mass or more, even more preferably 55% by mass or more, particularly preferably 60% by mass or more can be

<(D) Curing accelerator>
The resin composition of the present invention may further contain (D) a curing accelerator as an optional component. (D) Curing accelerator has a function of accelerating curing of (C) epoxy resin.

(D) The curing accelerator is not particularly limited, but for example, phosphorus-based curing accelerator, urea-based curing accelerator, amine-based curing accelerator, imidazole-based curing accelerator, guanidine-based curing accelerator, A metal-based curing accelerator and the like are included. Among them, phosphorus-based curing accelerators, amine-based curing accelerators, imidazole-based curing accelerators, and metal-based curing accelerators are preferable, and amine-based curing accelerators and imidazole-based curing accelerators are particularly preferable. The curing accelerator may be used singly or in combination of two or more.

Phosphorus curing accelerators include, for example, tetrabutylphosphonium bromide, tetrabutylphosphonium chloride, tetrabutylphosphonium acetate, tetrabutylphosphonium decanoate, tetrabutylphosphonium laurate, bis(tetrabutylphosphonium) pyromellitate, tetrabutylphosphonium hydro Aliphatic phosphonium salts such as genhexahydrophthalate, tetrabutylphosphonium cresol novolac trimer salt, di-tert-butylmethylphosphonium tetraphenylborate; methyltriphenylphosphonium bromide, ethyltriphenylphosphonium bromide, propyltriphenylphosphonium bromide, Butyltriphenylphosphonium bromide, benzyltriphenylphosphonium chloride, tetraphenylphosphonium bromide, p-tolyltriphenylphosphonium tetra-p-tolylborate, tetraphenylphosphonium tetraphenylborate, tetraphenylphosphonium tetra-p-tolylborate, triphenylethylphosphonium Tetraphenylborate, tris(3-methylphenyl)ethylphosphonium tetraphenylborate, tris(2-methoxyphenyl)ethylphosphonium tetraphenylborate, (4-methylphenyl)triphenylphosphonium thiocyanate, tetraphenylphosphoniumthiocyanate, butyltriphenylphosphonium Aromatic phosphonium salts such as thiocyanate; Aromatic phosphine/borane complexes such as triphenylphosphine/triphenylborane; Aliphatic phosphines such as -tert-butylphosphine, trioctylphosphine, di-tert-butyl(2-butenyl)phosphine, di-tert-butyl(3-methyl-2-butenyl)phosphine, tricyclohexylphosphine; dibutylphenylphosphine , di-tert-butylphenylphosphine, methyldiphenylphosphine, ethyldiphenylphosphine, butyldiphenylphosphine, diphenylcyclohexylphosphine, triphenylphosphine, tri-o-tolylphosphine, tri-m-tolylphosphine, tri-p-tolylphosphine, Tris(4-ethylphenyl)phosphine, Tris(4-propylphenyl)phosphine, Tris(4-isopropylphenyl)phosphine, Tris(4-butylphenyl)phosphine, Tris(4-tert-butylphenyl)phosphine, Tris(2 ,4-dimethylphenyl)phosphine, tris(2,5-dimethylphenyl)phosphine, tris(2,6-dimethylphenyl)phosphine, tris(3,5-dimethylphenyl)phosphine, tris(2,4,6-trimethyl phenyl)phosphine, tris(2,6-dimethyl-4-ethoxyphenyl)phosphine, tris(2-methoxyphenyl)phosphine, tris(4-methoxyphenyl)phosphine, tris(4-ethoxyphenyl)phosphine, tris(4- tert-butoxyphenyl)phosphine, diphenyl-2-pyridylphosphine, 1,2-bis(diphenylphosphino)ethane, 1,3-bis(diphenylphosphino)propane, 1,4-bis(diphenylphosphino)butane, aromatic phosphines such as 1,2-bis(diphenylphosphino)acetylene and 2,2'-bis(diphenylphosphino)diphenyl ether;

Urea-based curing accelerators include, for example, 1,1-dimethylurea; 1,1,3-trimethylurea, 3-ethyl-1,1-dimethylurea, 3-cyclohexyl-1,1-dimethylurea, 3- Aliphatic dimethylurea such as cyclooctyl-1,1-dimethylurea; 3-phenyl-1,1-dimethylurea, 3-(4-chlorophenyl)-1,1-dimethylurea, 3-(3,4-dichlorophenyl )-1,1-dimethylurea, 3-(3-chloro-4-methylphenyl)-1,1-dimethylurea, 3-(2-methylphenyl)-1,1-dimethylurea, 3-(4- methylphenyl)-1,1-dimethylurea, 3-(3,4-dimethylphenyl)-1,1-dimethylurea, 3-(4-isopropylphenyl)-1,1-dimethylurea, 3-(4- methoxyphenyl)-1,1-dimethylurea, 3-(4-nitrophenyl)-1,1-dimethylurea, 3-[4-(4-methoxyphenoxy)phenyl]-1,1-dimethylurea, 3- [4-(4-chlorophenoxy)phenyl]-1,1-dimethylurea, 3-[3-(trifluoromethyl)phenyl]-1,1-dimethylurea, N,N-(1,4-phenylene) Aromatic dimethylurea such as bis(N',N'-dimethylurea), N,N-(4-methyl-1,3-phenylene)bis(N',N'-dimethylurea) [toluenebisdimethylurea] etc.

Examples of amine curing accelerators include trialkylamines such as triethylamine and tributylamine, 4-dimethylaminopyridine (DMAP), benzyldimethylamine, 2,4,6-tris(dimethylaminomethyl)phenol, 1, 8-diazabicyclo(5,4,0)-undecene, etc., and 4-dimethylaminopyridine is preferred.

Examples of imidazole curing accelerators include 2-methylimidazole, 2-undecylimidazole, 2-heptadecylimidazole, 1,2-dimethylimidazole, 2-ethyl-4-methylimidazole, 1,2-dimethylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2-phenyl-4-methylimidazole, 1-benzyl-2-methylimidazole, 1-benzyl-2-phenylimidazole, 1-cyanoethyl-2-methylimidazole, 1-cyanoethyl-2-undecylimidazole, 1-cyanoethyl-2-ethyl-4-methylimidazole, 1-cyanoethyl-2-phenylimidazole, 1-cyanoethyl-2-undecylimidazolium trimellitate, 1-cyanoethyl- 2-phenylimidazolium trimellitate, 2,4-diamino-6-[2'-methylimidazolyl-(1')]-ethyl-s-triazine, 2,4-diamino-6-[2'-undecyl imidazolyl-(1′)]-ethyl-s-triazine, 2,4-diamino-6-[2′-ethyl-4′-methylimidazolyl-(1′)]-ethyl-s-triazine, 2,4- Diamino-6-[2'-methylimidazolyl-(1')]-ethyl-s-triazine isocyanurate, 2-phenylimidazole isocyanurate, 2-phenyl-4,5-dihydroxymethylimidazole, 2- Phenyl-4-methyl-5-hydroxymethylimidazole, 2,3-dihydro-1H-pyrrolo[1,2-a]benzimidazole, 1-dodecyl-2-methyl-3-benzylimidazolium chloride, 2-methylimidazoline , 2-phenylimidazoline and other imidazole compounds, and adducts of imidazole compounds and epoxy resins.

As the imidazole-based curing accelerator, a commercially available product may be used, such as "P200-H50" manufactured by Mitsubishi Chemical Corporation.

Guanidine curing accelerators include, for example, dicyandiamide, 1-methylguanidine, 1-ethylguanidine, 1-cyclohexylguanidine, 1-phenylguanidine, 1-(o-tolyl)guanidine, dimethylguanidine, diphenylguanidine, trimethylguanidine, Tetramethylguanidine, Pentamethylguanidine, 1,5,7-triazabicyclo[4.4.0]dec-5-ene, 7-methyl-1,5,7-triazabicyclo[4.4.0] Dec-5-ene, 1-methylbiguanide, 1-ethylbiguanide, 1-n-butylbiguanide, 1-n-octadecylbiguanide, 1,1-dimethylbiguanide, 1,1-diethylbiguanide, 1-cyclohexylbiguanide, 1 -allylbiguanide, 1-phenylbiguanide, 1-(o-tolyl)biguanide and the like.

Metal-based curing accelerators include, for example, organometallic complexes or organometallic salts of metals such as cobalt, copper, zinc, iron, nickel, manganese, and tin. Specific examples of organometallic complexes include organocobalt complexes such as cobalt (II) acetylacetonate and cobalt (III) acetylacetonate, organocopper complexes such as copper (II) acetylacetonate, and zinc (II) acetylacetonate. and the like, organic iron complexes such as iron (III) acetylacetonate, organic nickel complexes such as nickel (II) acetylacetonate, and organic manganese complexes such as manganese (II) acetylacetonate. Examples of organic metal salts include zinc octoate, tin octoate, zinc naphthenate, cobalt naphthenate, tin stearate, and zinc stearate.

The content of the (D) curing accelerator in the resin composition is not particularly limited, but when the non-volatile components other than the (B) inorganic filler in the resin composition are 100% by mass, it is preferably It is 5% by mass or less, more preferably 2% by mass or less, still more preferably 1% by mass or less, and particularly preferably 0.5% by mass or less. The lower limit of the content of the (D) curing accelerator in the resin composition is not particularly limited, but when the non-volatile components other than the (B) inorganic filler in the resin composition are 100% by mass, For example, 0% by mass or more, 0.0001% by mass or more, 0.001% by mass or more, 0.01% by mass or more, 0.1% by mass or more, 0.2% by mass or more, 0.3% by mass or more, etc. obtain.

<(E) Other Additives>
The resin composition of the present invention may further contain optional additives as non-volatile components. Examples of such additives include organic fillers such as rubber particles, polyamide fine particles, and silicone particles; Thermoplastic resins such as ether ether ketone resins and polyester resins; Organometallic compounds such as organic copper compounds, organic zinc compounds, and organic cobalt compounds; phthalocyanine blue, phthalocyanine green, iodine green, diazo yellow, crystal violet, titanium oxide, carbon Coloring agents such as black; polymerization inhibitors such as hydroquinone, catechol, pyrogallol, and phenothiazine; leveling agents such as silicone-based leveling agents and acrylic polymer-based leveling agents; thickeners such as bentone and montmorillonite; Antifoaming agents such as antifoaming agents, fluorine antifoaming agents, and vinyl resin antifoaming agents; UV absorbers such as benzotriazole UV absorbers; adhesion improvers such as urea silane; triazole adhesion imparting agents , tetrazole-based adhesion-imparting agents, triazine-based adhesion-imparting agents; antioxidants such as hindered phenol-based antioxidants and hindered amine-based antioxidants; fluorescent brighteners such as stilbene derivatives; Surfactants such as surfactants and silicone surfactants; Flame retardants such as flame retardants and inorganic flame retardants (for example, antimony trioxide) can be used. One of the additives may be used alone, or two or more of them may be used in combination at an arbitrary ratio. (E) The content of other additives can be appropriately set by those skilled in the art.

<(F) Organic solvent>
The resin composition of the present invention may further contain an arbitrary organic solvent as a volatile component in addition to the non-volatile component described above. As the (F) organic solvent, a known one can be used as appropriate, and the type thereof is not particularly limited. (F) Examples of organic solvents include ketone solvents such as acetone, methyl ethyl ketone, methyl isobutyl ketone, and cyclohexanone; ester solvents such as butyrolactone; ether solvents such as tetrahydropyran, tetrahydrofuran, 1,4-dioxane, diethyl ether, diisopropyl ether, dibutyl ether, and diphenyl ether; alcohol solvents such as methanol, ethanol, propanol, butanol, and ethylene glycol; Ether ester solvents such as 2-ethoxyethyl acetate, propylene glycol monomethyl ether acetate, diethylene glycol monoethyl ether acetate, ethyl diglycol acetate, γ-butyrolactone, methyl methoxypropionate; methyl lactate, ethyl lactate, 2-hydroxyisobutyric acid ester alcohol solvents such as methyl; ether alcohol solvents such as 2-methoxypropanol, 2-methoxyethanol, 2-ethoxyethanol, propylene glycol monomethyl ether, diethylene glycol monobutyl ether (butyl carbitol); N,N-dimethylformamide, Amide solvents such as N,N-dimethylacetamide and N-methyl-2-pyrrolidone; sulfoxide solvents such as dimethylsulfoxide; nitrile solvents such as acetonitrile and propionitrile; hexane, cyclopentane, cyclohexane, methylcyclohexane and the like Aliphatic hydrocarbon solvents; aromatic hydrocarbon solvents such as benzene, toluene, xylene, ethylbenzene, trimethylbenzene, and the like can be mentioned. (F) The organic solvent may be used singly or in combination of two or more at any ratio. In one embodiment, the amount of the organic solvent (F) is preferably as small as possible (for example, when the non-volatile component in the resin composition is 100% by mass, it is 0.5% by mass or less, 0.1% by mass or less, 0.5% by mass or less, 0.1% by mass or less, 01% by mass or less), and it is particularly preferable not to contain them.

<Method for producing resin composition>
The resin composition of the present invention is, for example, placed in any reaction vessel (A) a curing agent, (B) an inorganic filler, optionally (C) an epoxy resin, optionally (D) a curing accelerator, optionally (E) other additives and, if necessary, (F) an organic solvent may be added in any order and/or partly or wholly at the same time and mixed. Also, during the process of adding and mixing each component, the temperature can be set appropriately, and heating and/or cooling may be performed temporarily or over time. Moreover, you may stir or shake in the process of adding and mixing each component. In addition, during or after adding and mixing each component, the resin composition may be stirred using a stirring device such as a mixer to uniformly disperse.

<Characteristics of resin composition>
The resin composition of the present invention is a resin composition containing (A) a curing agent and (B) an inorganic filler, wherein the component (A) contains (A-1) a hydroxyl group-containing siloxane compound, and (A -1) The content of the component is less than 5% by mass when the non-volatile components other than the component (B) in the resin composition are 100% by mass, and the content of the component (B) is in the resin composition When all the non-volatile components are 100% by mass, since it is 60% by mass or more, the occurrence of flow marks after molding and warping can be suppressed, and a cured product with excellent adhesion to a thermal peeling tape can be obtained. Obtainable.

In one embodiment, since the cured product of the resin composition of the present invention can suppress warping, a sample substrate including a silicon wafer and a cured product layer of the resin composition is prepared, for example, as in Test Example 1 below. , when the warp amount of the sample substrate at 25° C. is measured according to JEITA EDX-7311-24, the warp amount can be less than 3 mm.

In one embodiment, since the cured product of the resin composition of the present invention is excellent in adhesiveness to a thermal peeling tape, a sample substrate containing a silicon wafer and a resin composition is prepared, Even when the sample substrate is left at 23° C. for 30 minutes, no peeling occurs between the thermal peeling tape and the resin composition.

In one embodiment, the cured product of the resin composition of the present invention can suppress the generation of flow marks after molding. Therefore, for example, as in Test Example 3 below, a sample is prepared and the appearance of the resin composition layer is evaluated. When observed, the area occupied by flow marks can be less than 20% of the entire surface of the resin composition layer.

<Application of resin composition>
The resin composition of the present invention may contain (C) an epoxy resin, or may be mixed with (C) an epoxy resin before use. Hereinafter, the resin composition of the present invention containing (C) an epoxy resin or a resin composition obtained by mixing the resin composition of the present invention with (C) an epoxy resin is referred to as an "epoxy resin composition". Therefore, the resin composition of the present invention can be used as it is or by mixing with (C) epoxy resin for the same applications as the epoxy resin composition described below.

Due to the advantages described above, the cured epoxy resin composition of the present invention is particularly useful for sealing layers and insulating layers of semiconductors. Therefore, the epoxy resin composition in the present invention can be used as a resin composition for semiconductor encapsulation or an insulating layer.

For example, the epoxy resin composition in the present invention includes a resin composition for forming an insulating layer of a semiconductor chip package (a resin composition for an insulating layer of a semiconductor chip package) and a circuit board (printed wiring board). ) can be suitably used as a resin composition for forming an insulating layer (a resin composition for an insulating layer of a circuit board).

Further, for example, the epoxy resin composition in the present invention can be suitably used as a resin composition for sealing a semiconductor chip of a semiconductor chip package (resin composition for semiconductor chip sealing).

Examples of semiconductor chip packages to which the sealing layer or insulating layer formed of the cured epoxy resin composition of the present invention can be applied include FC-CSP, MIS-BGA package, ETS-BGA package, and Fan-out type WLP. (wafer level package), fan-in type WLP, fan-out type PLP (panel level package), and fan-in type PLP.

Further, the epoxy resin composition in the present invention may be used as an underfill material, for example, as a material for MUF (Molding Under Filling) used after connecting a semiconductor chip to a substrate.

Furthermore, the epoxy resin composition in the present invention includes resin sheets, sheet-like laminate materials such as prepreg, liquid materials such as resin inks for solder resists, etc., die bonding materials, hole-filling resins, component-embedding resins, etc. can be used for a wide range of applications.

<Resin sheet>
The resin sheet of the present invention has a support and a resin composition layer provided on the support. The resin composition layer is a layer containing the resin composition of the present invention as an epoxy resin composition. That is, when forming the resin composition layer, the resin composition of the present invention containing (C) an epoxy resin or the resin composition obtained by mixing the resin composition of the present invention with (C) an epoxy resin is used. use.

The thickness of the resin composition layer is preferably 600 µm or less, more preferably 500 µm or less, from the viewpoint of thinning. The lower limit of the thickness of the resin composition layer is preferably 1 µm or more, 5 µm or more, more preferably 10 µm or more, still more preferably 50 µm or more, and particularly preferably 100 µm or more.

The thickness of the cured product obtained by curing the resin composition layer is preferably 600 μm or less, more preferably 500 μm or less. The lower limit of the thickness of the cured product is preferably 1 µm or more, 5 µm or more, more preferably 10 µm or more, still more preferably 50 µm or more, and particularly preferably 100 µm or more.

Examples of the support include a film made of a plastic material, a metal foil, and a release paper, and a film made of a plastic material and a metal foil are preferable.

When a film made of a plastic material is used as the support, examples of the plastic material include polyethylene terephthalate (hereinafter sometimes abbreviated as "PET") and polyethylene naphthalate (hereinafter sometimes abbreviated as "PEN"). Polycarbonate (hereinafter sometimes abbreviated as "PC"); Acrylic polymers such as polymethyl methacrylate (hereinafter sometimes abbreviated as "PMMA"); Cyclic polyolefins; Triacetyl cellulose (hereinafter polyether sulfide (hereinafter sometimes abbreviated as "PES"); polyether ketone; polyimide; Among them, polyethylene terephthalate and polyethylene naphthalate are preferable, and inexpensive polyethylene terephthalate is particularly preferable.

When a metal foil is used as the support, examples of the metal foil include copper foil and aluminum foil. Among them, copper foil is preferable. As the copper foil, a foil made of a single metal of copper may be used, and a foil made of an alloy of copper and other metals (for example, tin, chromium, silver, magnesium, nickel, zirconium, silicon, titanium, etc.) may be used. may be used.

The support may be subjected to matte treatment, corona treatment, antistatic treatment, or the like on the surface to be bonded to the resin composition layer.

Further, as the support, a support with a release layer having a release layer on the surface to be bonded to the resin composition layer may be used. The release agent used in the release layer of the release layer-attached support includes, for example, one or more release agents selected from the group consisting of alkyd resins, polyolefin resins, urethane resins, and silicone resins. . Examples of commercially available release agents include alkyd resin-based release agents such as “SK-1”, “AL-5” and “AL-7” manufactured by Lintec. Examples of the release layer-attached support include "Lumirror T60" manufactured by Toray Industries, Inc.; "Purex" manufactured by Teijin Limited; and "Unipeel" manufactured by Unitika.

The thickness of the support is preferably in the range of 5 μm to 75 μm, more preferably in the range of 10 μm to 60 μm. When a release layer-attached support is used, the thickness of the release layer-attached support as a whole is preferably within the above range.

The resin sheet can be produced, for example, by coating an epoxy resin composition on a support using a coating device such as a die coater. Moreover, if necessary, the epoxy resin composition may be dissolved in an organic solvent to prepare a resin varnish, and the resin sheet may be produced by applying the resin varnish. By using an organic solvent, the viscosity can be adjusted and the coatability can be improved. When an epoxy resin composition or resin varnish containing an organic solvent is used, the epoxy resin composition or resin varnish is usually dried after coating to form a resin composition layer.

Drying may be carried out by a known method such as heating or blowing hot air. The drying conditions are such that the content of the organic solvent in the resin composition layer is usually 10% by mass or less, preferably 5% by mass or less. Depending on the boiling point of the organic solvent in the epoxy resin composition or resin varnish, for example, when using an epoxy resin composition or resin varnish containing 30% by mass to 60% by mass of an organic solvent, the temperature is 50° C. to 150° C. for 3 minutes. A resin composition layer can be formed by drying for ~10 minutes.

The resin sheet may contain arbitrary layers other than the support and the resin composition layer, if necessary. For example, in the resin sheet, the surface of the resin composition layer that is not bonded to the support (that is, the surface opposite to the support) may be provided with a protective film conforming to the support. The thickness of the protective film is, for example, 1 μm to 40 μm. The protective film can prevent dust from adhering to the surface of the resin composition layer and scratches on the surface of the resin composition layer. When the resin sheet has a protective film, the resin sheet can be used by peeling off the protective film. In addition, the resin sheet can be wound into a roll and stored.

A resin sheet can be suitably used for forming an insulating layer in the manufacture of a semiconductor chip package (an insulating resin sheet for a semiconductor chip package). For example, the resin sheet can be used to form an insulating layer of a circuit board (resin sheet for insulating layer of circuit board). Examples of packages using such substrates include FC-CSP, MIS-BGA packages, and ETS-BGA packages.

In addition, the resin sheet can be suitably used for sealing semiconductor chips (semiconductor chip sealing resin sheet). Applicable semiconductor chip packages include, for example, Fan-out type WLP, Fan-in type WLP, Fan-out type PLP, Fan-in type PLP and the like.

Also, the resin sheet may be used as a material for the MUF that is used after connecting the semiconductor chip to the substrate.

Furthermore, the resin sheet can be used in a wide range of other applications that require high insulation reliability. For example, a resin sheet can be suitably used to form an insulating layer of a circuit board such as a printed wiring board.

<Circuit board>
The circuit board of the present invention includes an insulating layer formed from a cured epoxy resin composition obtained from the resin composition of the present invention. This circuit board can be manufactured, for example, by a manufacturing method including the following steps (1) and (2).
(1) A step of forming a resin composition layer of an epoxy resin composition on a substrate using the resin composition of the present invention.
(2) A step of thermosetting the resin composition layer to form an insulating layer.

In step (1), a substrate is prepared. Examples of base materials include substrates such as glass epoxy substrates, metal substrates (stainless steel, cold-rolled steel plate (SPCC), etc.), polyester substrates, polyimide substrates, BT resin substrates, and thermosetting polyphenylene ether substrates. Moreover, the base material may have a metal layer such as a copper foil on the surface as part of the base material. For example, a substrate having peelable first and second metal layers on both surfaces may be used. When such a substrate is used, a conductor layer as a wiring layer capable of functioning as circuit wiring is usually formed on the surface of the second metal layer opposite to the first metal layer. As a substrate having such a metal layer, for example, an ultra-thin copper foil with a carrier copper foil "Micro Thin" manufactured by Mitsui Kinzoku Mining Co., Ltd. can be used.

Also, a conductor layer may be formed on one or both surfaces of the substrate. In the following description, a member including a base material and a conductor layer formed on the surface of the base material may be referred to as a "wiring layer-attached base material" as appropriate. The conductor material contained in the conductor layer is, for example, one selected from the group consisting of gold, platinum, palladium, silver, copper, aluminum, cobalt, chromium, zinc, nickel, titanium, tungsten, iron, tin and indium. Materials containing the above metals can be mentioned. As the conductor material, a single metal may be used, or an alloy may be used. Examples of alloys include alloys of two or more metals selected from the above group (eg, nickel-chromium alloys, copper-nickel alloys and copper-titanium alloys). Among them, chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver or copper as single metals; and nickel-chromium alloys as alloys , a copper-nickel alloy, and a copper-titanium alloy; are preferred. Among them, single metals of chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver or copper; and nickel-chromium alloys; are more preferred, and single metals of copper are particularly preferred.

The conductor layer may be patterned, for example, to function as a wiring layer. At this time, the line (circuit width) / space (width between circuits) ratio of the conductor layer is not particularly limited, but is preferably 20/20 μm or less (that is, the pitch is 40 μm or less), more preferably 10/10 μm or less, and further It is preferably 5/5 μm or less, more preferably 1/1 μm or less, and particularly preferably 0.5/0.5 μm or more. The pitch need not be the same throughout the conductor layer. The minimum pitch of the conductor layers may be, for example, 40 μm or less, 36 μm or less, or 30 μm or less.

The thickness of the conductor layer is preferably 3 μm to 35 μm, more preferably 5 μm to 30 μm, even more preferably 10 μm to 20 μm, particularly preferably 15 μm to 20 μm, depending on the design of the circuit board.

The conductor layer is formed by, for example, a process of laminating a dry film (photosensitive resist film) on a base material, and performing pattern drying by exposing and developing the dry film under predetermined conditions using a photomask to form a pattern. It can be formed by a method including a step of obtaining a film, a step of forming a conductor layer by a plating method such as electroplating using the developed patterned dry film as a plating mask, and a step of peeling off the patterned dry film. As the dry film, a photosensitive dry film made of a photoresist composition can be used. For example, a dry film made of a resin such as a novolak resin or an acrylic resin can be used. The conditions for laminating the substrate and the dry film may be the same as the conditions for laminating the substrate and the resin sheet, which will be described later. Stripping of the dry film can be carried out using, for example, an alkaline stripping solution such as sodium hydroxide solution.

After preparing the substrate, a resin composition layer is formed on the substrate. When a conductor layer is formed on the surface of the substrate, the resin composition layer is preferably formed so that the conductor layer is embedded in the resin composition layer.

Formation of the resin composition layer is performed, for example, by laminating a resin sheet and a substrate. This lamination can be performed, for example, by bonding the resin composition layer to the substrate by thermocompression bonding the resin sheet to the substrate from the support side. Examples of the member for thermocompression bonding the resin sheet to the substrate (hereinafter sometimes referred to as "thermocompression member") include heated metal plates (such as SUS end plates) and metal rolls (such as SUS rolls). be done. Instead of pressing the thermocompression member directly onto the resin sheet, it is preferable to press the resin sheet through an elastic material such as heat-resistant rubber so that the resin sheet can sufficiently follow the uneven surface of the substrate.

Lamination of the base material and the resin sheet may be carried out, for example, by a vacuum lamination method. In the vacuum lamination method, the thermocompression bonding temperature is preferably in the range of 60°C to 160°C, more preferably 80°C to 140°C. The thermocompression pressure is preferably in the range of 0.098 MPa to 1.77 MPa, more preferably 0.29 MPa to 1.47 MPa. The thermocompression bonding time is preferably in the range of 20 seconds to 400 seconds, more preferably 30 seconds to 300 seconds. Lamination is preferably carried out under reduced pressure conditions of 13 hPa or less.

After lamination, the laminated resin sheets may be smoothed under normal pressure (atmospheric pressure), for example, by pressing a thermocompression member from the support side. Pressing conditions for the smoothing treatment may be the same as the thermocompression bonding conditions for the lamination described above. Lamination and smoothing may be performed continuously using a vacuum laminator.

Formation of the resin composition layer can be performed by, for example, a compression molding method. As the molding conditions, the same conditions as in the method of forming the resin composition layer in the step of forming the sealing layer of the semiconductor chip package, which will be described later, may be adopted.

After forming the resin composition layer on the substrate, the resin composition layer is thermally cured to form an insulating layer. The thermosetting conditions for the resin composition layer vary depending on the type of resin composition, but the curing temperature is usually in the range of 120°C to 240°C (preferably in the range of 150°C to 220°C, more preferably in the range of 170°C to 200°C). range), and the curing time is in the range of 5 minutes to 120 minutes (preferably 10 minutes to 100 minutes, more preferably 15 minutes to 90 minutes).

Prior to thermal curing of the resin composition layer, the resin composition layer may be subjected to a preheating treatment of heating at a temperature lower than the curing temperature. For example, prior to thermosetting the resin composition layer, the resin composition layer is usually heated at a temperature of 50 ° C. or higher and lower than 120 ° C. (preferably 60 ° C. or higher and 110 ° C. or lower, more preferably 70 ° C. or higher and 100 ° C. or lower). may be preheated for usually 5 minutes or more (preferably 5 minutes to 150 minutes, more preferably 15 minutes to 120 minutes).

A circuit board having an insulating layer can be manufactured in the manner described above. Moreover, the method for manufacturing the circuit board may further include an arbitrary step.
For example, when a circuit board is manufactured using a resin sheet, the method for manufacturing the circuit board may include a step of peeling off the support of the resin sheet. The support may be peeled off before heat curing of the resin composition layer, or may be peeled off after heat curing of the resin composition layer.

The method of manufacturing the circuit board may include, for example, a step of polishing the surface of the insulating layer after forming the insulating layer. A polishing method is not particularly limited. For example, the surface of the insulating layer can be polished using a surface grinder.

The method of manufacturing the circuit board may include, for example, the step (3) of connecting the conductor layers between layers, for example, the step of drilling holes in the insulating layer. As a result, holes such as via holes and through holes can be formed in the insulating layer. Examples of methods for forming via holes include laser irradiation, etching, and mechanical drilling. The size and shape of the via hole may be appropriately determined according to the design of the circuit board. In step (3), interlayer connection may be performed by polishing or grinding the insulating layer.

After forming the via hole, it is preferable to perform a step of removing smear in the via hole. This process is sometimes called a desmear process. For example, when the conductive layer is formed on the insulating layer by a plating process, the via holes may be subjected to a wet desmear treatment. Further, when the conductor layer is formed on the insulating layer by a sputtering process, a dry desmear process such as a plasma treatment process may be performed. Furthermore, the insulating layer may be roughened by a desmear process.

Further, the insulating layer may be roughened before forming the conductor layer on the insulating layer. According to this roughening treatment, the surface of the insulating layer including the inside of the via hole is usually roughened. As the roughening treatment, either dry or wet roughening treatment may be performed. Examples of dry roughening treatment include plasma treatment and the like. Moreover, examples of wet roughening treatment include a method in which swelling treatment with a swelling liquid, roughening treatment with an oxidizing agent, and neutralization treatment with a neutralizing liquid are performed in this order.

After forming the via holes, a conductor layer may be formed on the insulating layer. By forming a conductor layer at the position where the via hole is formed, the newly formed conductor layer and the conductor layer on the surface of the base material are electrically connected to each other, thereby performing interlayer connection. Methods for forming the conductor layer include, for example, plating, sputtering, vapor deposition, etc. Among them, plating is preferable. In a preferred embodiment, the surface of the insulating layer is plated by an appropriate method such as a semi-additive method or a full-additive method to form a conductor layer having a desired wiring pattern. Moreover, when the support in the resin sheet is a metal foil, a conductor layer having a desired wiring pattern can be formed by a subtractive method. The material of the conductor layer to be formed may be a single metal or an alloy. Moreover, this conductor layer may have a single layer structure, or may have a multi-layer structure including two or more layers of different kinds of materials.

An example embodiment of forming a conductor layer on an insulating layer will now be described in detail. A plating seed layer is formed on the surface of the insulating layer by electroless plating. Next, a mask pattern is formed on the formed plating seed layer to expose a portion of the plating seed layer corresponding to a desired wiring pattern. After forming an electrolytic plating layer on the exposed plating seed layer by electrolytic plating, the mask pattern is removed. After that, the unnecessary plating seed layer is removed by a treatment such as etching to form a conductor layer having a desired wiring pattern. The dry film used for forming the mask pattern when forming the conductor layer is the same as the dry film described above.

The circuit board manufacturing method may include a step (4) of removing the base material. By removing the substrate, a circuit board having an insulating layer and a conductor layer embedded in this insulating layer is obtained. This step (4) can be performed, for example, when a base material having a peelable metal layer is used.

<Semiconductor chip package>
A semiconductor chip package according to a first embodiment of the present invention includes the circuit board described above and a semiconductor chip mounted on the circuit board. This semiconductor chip package can be manufactured by bonding a semiconductor chip to a circuit board.

Any condition that allows conductor connection between the terminal electrodes of the semiconductor chip and the circuit wiring of the circuit board can be adopted as the bonding condition of the circuit board and the semiconductor chip. For example, conditions used in flip-chip mounting of semiconductor chips can be employed. Alternatively, for example, the semiconductor chip and the circuit board may be bonded via an insulating adhesive.

As an example of the bonding method, there is a method of crimping the semiconductor chip to the circuit board. As for the crimping conditions, the crimping temperature is usually in the range of 120° C. to 240° C. (preferably 130° C. to 200° C., more preferably 140° C. to 180° C.), and the crimping time is usually in the range of 1 second to 60 seconds. (preferably 5 seconds to 30 seconds).

Another example of the bonding method is a method of reflowing and bonding a semiconductor chip to a circuit board. The reflow conditions may range from 120.degree. C. to 300.degree.

After bonding the semiconductor chip to the circuit board, the semiconductor chip may be filled with a mold underfill material. As the mold underfill material, the resin composition described above may be used, or the resin sheet described above may be used.

A semiconductor chip package according to a second embodiment of the present invention includes a semiconductor chip and a cured product of the resin composition sealing the semiconductor chip. In such a semiconductor chip package, the cured resin composition usually functions as a sealing layer. As a semiconductor chip package according to the second embodiment, for example, a fan-out type WLP can be used.

A method for manufacturing such a semiconductor chip package includes:
(A) a step of laminating a temporary fixing film on a substrate;
(B) temporarily fixing the semiconductor chip on the temporary fixing film;
(C) forming a sealing layer on the semiconductor chip;
(D) a step of peeling the substrate and the temporary fixing film from the semiconductor chip;
(E) forming a rewiring formation layer as an insulating layer on the surface of the semiconductor chip from which the substrate and the temporary fixing film have been removed;
(F) forming a rewiring layer as a conductor layer on the rewiring forming layer;
(G) forming a solder resist layer on the rewiring layer;
including. Further, the method for manufacturing the semiconductor chip package includes:
(H) A step of dicing the plurality of semiconductor chip packages into individual semiconductor chip packages to individualize them.

(Step (A))
Step (A) is a step of laminating a temporary fixing film on a substrate. The conditions for laminating the base material and the temporary fixing film may be the same as the conditions for laminating the base material and the resin sheet in the method for manufacturing a circuit board.

Examples of substrates include silicon wafers; glass wafers; glass substrates; metal substrates such as copper, titanium, stainless steel and cold-rolled steel plate (SPCC); FR-4 substrates and the like; A heat-cured substrate; a substrate made of bismaleimide triazine resin such as BT resin; and the like.

Any material that can be peeled off from the semiconductor chip and that can temporarily fix the semiconductor chip can be used for the temporary fixing film. Commercially available products include "Riva Alpha" manufactured by Nitto Denko Corporation.

(Step (B))
Step (B) is a step of temporarily fixing the semiconductor chip on the temporary fixing film. Temporary fixing of the semiconductor chip can be performed using a device such as a flip chip bonder, a die bonder, or the like. The layout and the number of semiconductor chips to be arranged can be appropriately set according to the shape and size of the temporary fixing film, the target production number of semiconductor chip packages, and the like. For example, the semiconductor chips may be arranged in a matrix of multiple rows and multiple columns and temporarily fixed.

(Step (C))
Step (C) is a step of forming a sealing layer on the semiconductor chip. The sealing layer is formed from a cured product of the resin composition described above. The encapsulation layer is usually formed by a method including the steps of forming a resin composition layer on the semiconductor chip and thermosetting the resin composition layer to form the encapsulation layer.

Formation of the resin composition layer is preferably carried out by a compression molding method. In the compression molding method, a semiconductor chip and a resin composition are usually placed in a mold, and pressure and, if necessary, heat are applied to the resin composition in the mold to form a resin composition layer covering the semiconductor chip.

A specific operation of the compression molding method can be, for example, as follows. An upper mold and a lower mold are prepared as molds for compression molding. Also, the resin composition is applied to the semiconductor chip temporarily fixed on the temporary fixing film as described above. The semiconductor chip coated with the resin composition is attached to the lower mold together with the substrate and the temporary fixing film. After that, the upper mold and the lower mold are clamped, and heat and pressure are applied to the resin composition for compression molding.

Further, the specific operation of the compression molding method may be, for example, as follows. An upper mold and a lower mold are prepared as molds for compression molding. A resin composition is placed on the lower mold. Also, the semiconductor chip is attached to the upper mold together with the base material and the temporary fixing film. Thereafter, the upper mold and the lower mold are clamped so that the resin composition placed on the lower mold is in contact with the semiconductor chip attached to the upper mold, and heat and pressure are applied to perform compression molding.

Molding conditions vary depending on the composition of the resin composition, and suitable conditions can be adopted so as to achieve good sealing. For example, the temperature of the mold during molding is preferably 70°C or higher, more preferably 80°C or higher, particularly preferably 90°C or higher, preferably 200°C or lower, more preferably 170°C or lower, and particularly preferably 150°C. It is below. The pressure applied during molding is preferably 1 MPa or higher, more preferably 3 MPa or higher, particularly preferably 5 MPa or higher, and preferably 50 MPa or lower, more preferably 30 MPa or lower, and particularly preferably 20 MPa or lower. The cure time is preferably 1 minute or more, more preferably 2 minutes or more, particularly preferably 3 minutes or more, and preferably 60 minutes or less, more preferably 30 minutes or less, and particularly preferably 20 minutes or less. After formation of the resin composition layer, the mold is usually removed. The mold may be removed before or after heat curing of the resin composition layer.

The resin composition layer may be formed by laminating a resin sheet and a semiconductor chip. For example, the resin composition layer can be formed on the semiconductor chip by thermocompression bonding the resin composition layer of the resin sheet and the semiconductor chip. The lamination of the resin sheet and the semiconductor chip can be carried out in the same manner as the lamination of the resin sheet and the base material in the circuit board manufacturing method, using the semiconductor chip instead of the base material.

After forming the resin composition layer on the semiconductor chip, the resin composition layer is thermally cured to obtain a sealing layer covering the semiconductor chip. As a result, the semiconductor chip is sealed with the cured product of the resin composition. The thermosetting conditions for the resin composition layer may be the same as the thermosetting conditions for the resin composition layer in the circuit board manufacturing method. Furthermore, before thermally curing the resin composition layer, the resin composition layer may be subjected to a preheating treatment of heating at a temperature lower than the curing temperature. As the processing conditions for this preheating treatment, the same conditions as those for the preheating treatment in the circuit board manufacturing method may be employed.

(Step (D))
Step (D) is a step of peeling off the substrate and the temporary fixing film from the semiconductor chip. As for the peeling method, it is desirable to employ an appropriate method according to the material of the temporary fixing film. Examples of the peeling method include a method of heating, foaming, or expanding the temporary fixing film to peel it. Moreover, as a peeling method, for example, a method of irradiating the temporary fixing film with ultraviolet rays through the base material to reduce the adhesive strength of the temporary fixing film and peel it off can be used.

In the method of peeling by heating, foaming or expanding the temporary fixing film, the heating conditions are usually 100° C. to 250° C. for 1 second to 90 seconds or 5 minutes to 15 minutes. In the method of peeling off the temporary fixing film by irradiating it with ultraviolet rays to reduce its adhesive strength, the irradiation dose of ultraviolet rays is usually 10 mJ/cm ² to 1000 mJ/cm ² .

(Step (E))
Step (E) is a step of forming a rewiring forming layer as an insulating layer on the surface of the semiconductor chip from which the substrate and the temporary fixing film have been removed.

Any insulating material can be used as the material of the rewiring formation layer. Among them, photosensitive resins and thermosetting resins are preferable from the viewpoint of easiness in manufacturing semiconductor chip packages. Moreover, you may use the resin composition of this invention as this thermosetting resin.

After the rewiring formation layer is formed, via holes may be formed in the rewiring formation layer for interlayer connection between the semiconductor chip and the rewiring layer.

In the method of forming a via hole when the material of the rewiring layer is a photosensitive resin, the surface of the rewiring layer is usually irradiated with an active energy ray through a mask pattern to irradiate the rewiring layer in the irradiated portion with light. Harden. Examples of active energy rays include ultraviolet rays, visible rays, electron beams, and X-rays, and ultraviolet rays are particularly preferred. The irradiation amount and irradiation time of ultraviolet rays can be appropriately set according to the photosensitive resin. The exposure method includes, for example, a contact exposure method in which the mask pattern is brought into close contact with the rewiring layer and exposed, and a non-contact exposure method in which the mask pattern is not brought into close contact with the rewiring layer and is exposed using parallel light rays. is mentioned.

After the rewiring layer is photo-cured, the rewiring layer is developed to remove the unexposed portions to form via holes. The development may be either wet development or dry development. The development method includes, for example, a dipping method, a paddle method, a spray method, a brushing method, a scraping method, and the like, and the paddle method is preferable from the viewpoint of resolution.

When the material of the rewiring formation layer is a thermosetting resin, the method of forming via holes includes, for example, laser irradiation, etching, mechanical drilling, and the like. Among them, laser irradiation is preferable. Laser irradiation can be performed using an appropriate laser processing machine using a light source such as a carbon dioxide laser, a UV-YAG laser, an excimer laser, or the like.

Although the shape of the via hole is not particularly limited, it is generally circular (substantially circular). The top diameter of the via hole is preferably 50 μm or less, more preferably 30 μm or less, still more preferably 20 μm or less. Here, the top diameter of the via hole means the diameter of the opening of the via hole on the surface of the rewiring layer.

(Step (F))
Step (F) is a step of forming a rewiring layer as a conductor layer on the rewiring forming layer. The method of forming the rewiring layer on the rewiring forming layer can be the same as the method of forming the conductor layer on the insulating layer in the method of manufacturing the circuit board. Alternatively, the steps (E) and (F) may be repeated to alternately build up the rewiring layers and the rewiring formation layers (build-up).

(Step (G))
Step (G) is a step of forming a solder resist layer on the rewiring layer. Any insulating material can be used as the material of the solder resist layer. Among them, photosensitive resins and thermosetting resins are preferable from the viewpoint of easiness in manufacturing semiconductor chip packages. Moreover, you may use the resin composition of this invention as a thermosetting resin.

Moreover, in the step (G), a bumping process for forming bumps may be performed as necessary. Bumping can be performed by a method such as solder balls or solder plating. Formation of via holes in the bumping process can be performed in the same manner as in step (E).

(Step (H))
The method for manufacturing a semiconductor chip package may include step (H) in addition to steps (A) to (G). Step (H) is a step of dicing a plurality of semiconductor chip packages into individual semiconductor chip packages to separate them into pieces. The method of dicing the semiconductor chip package into individual semiconductor chip packages is not particularly limited.

<Semiconductor device>
A semiconductor device includes a semiconductor chip package. Examples of semiconductor devices include electrical products (e.g., computers, mobile phones, smartphones, tablet devices, wearable devices, digital cameras, medical equipment, televisions, etc.) and vehicles (e.g., motorcycles, automobiles, trains, ships, etc.). and aircraft, etc.).

EXAMPLES Hereinafter, the present invention will be specifically described with reference to examples. The invention is not limited to these examples. In the following description, "parts" representing amounts mean "parts by mass" unless otherwise specified.

<Example 1>
Phenolic hydroxyl group-containing siloxane compound (manufactured by Shin-Etsu Chemical Co., Ltd. "KF-2201", hydroxyl value 38 mgKOH / g) 1 part, acid anhydride curing agent (manufactured by Shin Nippon Rika "HNA-100", acid anhydride equivalent 179 g / eq.) 8 parts, silica (average particle size 6.9 μm, specific surface area 3.4 m ² / g, surface-treated with Shin-Etsu Chemical Co., Ltd. “KBM5783”) 120 parts, bisphenol type epoxy resin (Nippon Steel Chemical & Materials Co., Ltd. "ZX1059", epoxy equivalent about 165 g / eq., 1:1 mixture of bisphenol A type epoxy resin and bisphenol F type epoxy resin) 7 parts, glycidylamine type epoxy resin ("630" manufactured by Mitsubishi Chemical Corporation, epoxy Equivalent weight of about 95 g / eq.) 5 parts, dicyclopentadiene type epoxy resin (manufactured by DIC "HP-7200L", epoxy equivalent weight of about 250 g / eq.) 2 parts, imidazole-based curing accelerator (manufactured by Shikoku Kasei Kogyo Co., Ltd. "1B2PZ , 1-benzyl-2-phenylimidazole) was uniformly dispersed using a mixer to prepare a resin composition.

<Example 2>
Resin in the same manner as in Example 1 except that the amount of the phenolic hydroxyl group-containing siloxane compound (manufactured by Shin-Etsu Chemical Co., Ltd. "KF-2201", hydroxyl value 38 mgKOH / g) was changed from 1 part to 0.5 parts. A composition was obtained.

<Example 3>
Instead of 120 parts of silica (average particle size 6.9 μm, specific surface area 3.4 m ² /g, surface-treated with “KBM5783” manufactured by Shin-Etsu Chemical Co., Ltd.), alumina (average particle size 6.0 μm, specific surface area 1.0 μm) was used. A resin composition was obtained in the same manner as in Example 1, except for using 165 parts of 7 m ² /g, surface-treated with "KBM573" manufactured by Shin-Etsu Chemical Co., Ltd.).

<Example 4>
Instead of 120 parts of silica (average particle size 6.9 μm, specific surface area 3.4 m ² /g, surface-treated with “KBM5783” manufactured by Shin-Etsu Chemical Co., Ltd.), alumina (average particle size 6.0 μm, specific surface area 1.0 μm) was used. A resin composition was obtained in the same manner as in Example 2, except for using 165 parts of 7 m ² /g, surface-treated with "KBM573" manufactured by Shin-Etsu Chemical Co., Ltd.).

<Example 5>
Phenolic hydroxyl group-containing siloxane compound (manufactured by Shin-Etsu Chemical Co., Ltd. "KF-2201", hydroxyl value 38 mgKOH / g) instead of 1 part, carbinol-type hydroxyl group-containing siloxane compound (manufactured by Shin-Etsu Chemical Co., Ltd. "KF-6002", hydroxyl group A resin composition was obtained in the same manner as in Example 1, except for using 0.5 parts of a 35 mg KOH/g).

<Example 6>
Phenolic hydroxyl group-containing siloxane compound (manufactured by Shin-Etsu Chemical Co., Ltd. "KF-2201", hydroxyl value 38 mgKOH / g) instead of 1 part, carbinol type hydroxyl group-containing siloxane compound (manufactured by Shin-Etsu Chemical Co., Ltd. "X-22-4039" A resin composition was obtained in the same manner as in Example 1, except that 0.5 part of , hydroxyl value 58 mgKOH/g) was used.

<Comparative Example 1>
Resin composition in the same manner as in Example 1 except that the amount of the phenolic hydroxyl group-containing siloxane compound (manufactured by Shin-Etsu Chemical Co., Ltd. "KF-2201", hydroxyl value 38 mgKOH / g) was changed from 1 part to 3 parts. got

<Comparative Example 2>
A resin composition was obtained in the same manner as in Example 1, except that the phenolic hydroxyl group-containing siloxane compound ("KF-2201" manufactured by Shin-Etsu Chemical Co., Ltd., hydroxyl value 38 mgKOH/g) was not used.

<Test Example 1: Evaluation of warpage>
On a 12-inch silicon wafer, the resin compositions prepared in Examples and Comparative Examples were compression-molded using a compression molding apparatus (mold temperature: 130°C, pressure: 6 MPa, cure time: 10 minutes) to obtain a thickness. A resin composition layer having a thickness of 300 μm was formed. After that, the resin composition layer was thermally cured by heating at 180° C. for 90 minutes. As a result, a sample substrate including a silicon wafer and a cured product layer of the resin composition was obtained. Using a shadow moiré measuring device (“Thermoire AXP” manufactured by Akorometrics), the amount of warpage at 25° C. of the sample substrate was measured. The measurement was performed in accordance with JEITA EDX-7311-24 of the Japan Electronics and Information Technology Industries Association standard. Specifically, a virtual plane calculated by the method of least squares of all data of the substrate surface in the measurement area is used as a reference plane, and the difference between the minimum value and the maximum value in the direction perpendicular to the reference plane is obtained as the amount of warpage. evaluated according to the standard.
"○": Warp amount less than 3 mm "×": Warp amount 3 mm or more

<Test Example 2: Evaluation of thermal release tape adhesion>
A thermal release tape (“Riva Alpha No. 3195V” manufactured by Nitto Denko Co., Ltd.), which has adhesiveness at room temperature and can be easily peeled off when heated, was attached to a 12-inch silicon wafer. The resin compositions prepared in Examples and Comparative Examples were compression molded using a compression molding apparatus (mold temperature: 130°C, pressure: 6 MPa, cure time: 10 minutes) to form a resin composition layer having a thickness of 300 µm. formed. A sample substrate containing the silicon wafer and the resin composition was thus obtained.
"○": When the sample substrate is left at 23 ° C. for 30 minutes and no peeling occurs between the thermal peeling tape and the resin composition "X": The sample substrate is left at 23 ° C. for 30 minutes and the thermal peeling tape and the resin composition When delamination occurs between

<Test Example 3: Evaluation of flow marks after molding>
On a 12-inch silicon wafer, the resin compositions prepared in Examples and Comparative Examples were compression-molded using a compression molding apparatus (mold temperature: 130°C, pressure: 6 MPa, cure time: 10 minutes) to obtain a thickness. A resin composition layer having a thickness of 300 μm was formed and used as a sample. After that, the appearance of the resin composition layer of the sample was observed and evaluated according to the following criteria.
"○": The area occupied by flow marks is less than 20% of the entire surface of the resin composition layer. "X": The area occupied by flow marks is 20% or more of the entire surface of the resin composition layer.

Table 1 below shows the non-volatile components and amounts used in the resin compositions of Examples and Comparative Examples, and the evaluation results of Test Examples.

From the above results, when using a resin composition containing (A-1) a hydroxyl group-containing siloxane compound and (B) an inorganic filler in a predetermined ratio, the occurrence of flow marks and warping after molding can be suppressed. , and a cured product having excellent adhesiveness to a heat-peeling tape can be obtained.

Claims (17)

A resin composition comprising (A) a curing agent, (B) an inorganic filler, and (C) an epoxy resin,
(A) component contains an acid anhydride-based curing agent and (A-1) a hydroxyl group-containing siloxane compound,
(A-1) component is the formula (1):

[In the formula, at least two of 2n+2 R ¹ and two R ² independently represent an optionally substituted monovalent hydrocarbon group having one or more hydroxyl groups, and the others independently represents an optionally substituted monovalent hydrocarbon group; or at least two of the 2n+2 R ¹ independently represent an optionally substituted monovalent hydrocarbon group having one or more hydroxyl groups and others independently represent an optionally substituted monovalent hydrocarbon group, and two R ² together represent one —O— and bond to each other to form a cyclic siloxane skeleton. Form. n represents an integer of 2 or more. ]
containing a siloxane compound represented by
The component (C) contains an epoxy resin that is liquid at a temperature of 20°C and an epoxy resin that is solid at a temperature of 20°C, and the mass ratio of the epoxy resin that is solid at a temperature of 20°C to the epoxy resin that is liquid at a temperature of 20°C ( solid epoxy resin/liquid epoxy resin) is 0.2 to 10,
The content of component (A-1) is 3% by mass to 20% by mass when all of component (A) is 100% by mass,
The content of the component (A-1) is 0.5% by mass or more and less than 5% by mass when the non-volatile components other than the component (B) in the resin composition are 100% by mass,
The content of component (B) is 60% by mass or more when all non-volatile components in the resin composition are 100% by mass,
A resin composition in which the content of component (C) is 10% by mass or more and 90% by mass or less when non-volatile components other than component (B) in the resin composition are taken as 100% by mass. 2. The resin composition according to claim 1 , wherein component (A-1) is a phenolic hydroxyl group-containing siloxane compound. 3. The resin composition according to claim 1 , wherein component (A-1) has a chain siloxane skeleton. 4. The resin composition according to any one of claims 1 to 3 , wherein component (A-1) has a hydroxyl value of 120 mgKOH/g or less. The resin composition according to any one of claims 1 to 4 , wherein component (B) is silica. The resin composition according to any one of claims 1 to 5 , wherein the content of component (B) is 70% by mass or more when all non-volatile components in the resin composition are taken as 100% by mass. 7. The resin composition according to claim 6 , wherein the content of component (B) is 80% by mass or more when all non-volatile components in the resin composition are taken as 100% by mass. The content ratio of component (B) to component (A-1) ((B) component/(A-1) component) is 50 to 1,000, according to any one of claims 1 to 7 . of the resin composition. The resin composition according to any one of claims 1 to 8 , for forming an insulating layer of a semiconductor chip package. The resin composition according to any one of claims 1 to 8 , for forming an insulating layer of a circuit board. The resin composition according to any one of claims 1 to 8 , for encapsulating a semiconductor chip in a semiconductor chip package. A cured product obtained from the resin composition according to any one of claims 1 to 11 . A resin sheet comprising a support and a resin composition layer containing the resin composition according to any one of claims 1 to 11 provided on the support. A circuit board comprising an insulating layer formed from a cured product obtained from the resin composition according to any one of claims 1 to 11 . A semiconductor chip package comprising the circuit board according to claim 14 and a semiconductor chip mounted on the circuit board. A semiconductor chip package comprising a semiconductor chip and a cured product obtained from the resin composition according to any one of claims 1 to 11 for sealing the semiconductor chip. A semiconductor device comprising the semiconductor chip package according to claim 15 or 16 .