Resin composition

Abstract

To provide a resin composition that yields a cured product having superior resin flatness, dielectric properties, and peel strength.SOLUTION: A resin composition comprises a radical-polymerizable resin A having a cyclic structure in its main skeleton, and di-t-amyl peroxide.SELECTED DRAWING: None

Description

[Technical field]

[0001] The present invention relates to a resin composition. The present invention further relates to a resin sheet, a cured product, a circuit board, and a semiconductor device obtained by using the resin composition. [Background technology]

[0002] As a manufacturing technique for circuit boards such as printed wiring boards and rewiring boards for semiconductor packages, a manufacturing method using a build-up method in which insulating layers and conductor layers are alternately stacked is known. As an insulating material used for such insulating layers, for example, Patent Document 1 discloses a resin composition containing a radical polymerizable compound. [Prior art documents] [Patent documents]

[0003] [Patent Document 1] JP 2017-71798 A Summary of the Invention [Problem to be solved by the invention]

[0004] In recent years, there has been a demand for further improvement in dielectric properties such as the dielectric constant and dielectric tangent of insulating layers, as well as further improvement in adhesion strength (peel strength) with a conductor layer. In addition, when an insulating layer is formed on a substrate having irregularities, the surface of the insulating layer opposite the substrate may follow the irregularities of the substrate, resulting in a decrease in flatness of the insulating layer.

[0005] An object of the present invention is to provide a resin composition which is capable of giving a cured product having excellent surface flatness (hereinafter also referred to as resin flatness) and exhibiting good dielectric properties and peel strength; a resin sheet containing the resin composition; and a circuit board and a semiconductor device which are provided with an insulating layer formed using the resin composition. [Means for solving the problem]

[0006] As a result of intensive research into the above-mentioned problems, the inventors have found that the above-mentioned problems can be solved by using a combination of a specific radical polymerizable resin and di-t-amyl peroxide, and have thus completed the present invention.

[0007] That is, the present invention includes the following. [1] A radical polymerizable resin A having a ring structure in its main skeleton, and A resin composition containing di-t-amyl peroxide. [2] The resin composition according to [1], wherein the radical polymerizable resin A contains two or more types of radical polymerizable resins. [3] The resin composition according to [1] or [2], wherein the radical polymerizable resin A contains at least a resin selected from the group consisting of a maleimide resin, a terminal double bond-modified polyphenylene ether resin, and a (meth)acrylic resin. [4] The resin composition according to any one of [1] to [3], wherein the radical polymerizable resin A contains a radical polymerizable resin having a molecular weight of 1,000 or less. [5] The resin composition according to any one of [1] to [4], wherein the radical polymerizable resin A comprises a radical polymerizable resin (A-1) having an active group equivalent of 250 g / eq. or more and a radical polymerizable resin (A-2) having an active group equivalent of less than 250 g / eq. [6] The resin composition according to [5], wherein the content of the radical polymerizable resin (A-2) is less than the content of the radical polymerizable resin (A-1). [7] The resin composition according to [5] or [6], wherein the content of the radical polymerizable resin (A-2) is 50% or less of the content of the radical polymerizable resin (A-1). [8] The resin composition according to any one of [1] to [7], wherein the content of the radical polymerizable resin A is 40 mass% or more when the resin component in the resin composition is 100 mass%. [9] The resin composition according to any one of [1] to [8], wherein the content of di-t-amyl peroxide is 0.1 mass% or more and 2.5 mass% or less, when the resin component in the resin composition is 100 mass%.

[10] The resin composition according to any one of [1] to [9], further comprising an inorganic filler.

[11] The resin composition according to

[10] , wherein the content of the inorganic filler is 30% by mass or more when the non-volatile components in the resin composition are 100% by mass.

[12] The resin composition according to any one of [1] to

[11] , further comprising a thermoplastic resin.

[13] The resin composition according to

[12] , wherein the content of the thermoplastic resin is 0.1% by mass or more and 5.0% by mass or less, when the resin component in the resin composition is 100% by mass.

[14] The resin composition according to any one of [1] to

[13] , which is for use in an insulating layer of a circuit board.

[15] A resin sheet comprising a support and a layer of the resin composition according to any one of [1] to

[14] provided on the support.

[16] The resin sheet according to

[15] , wherein the support is a thermoplastic resin film or a metal foil.

[17] A cured product of the resin composition according to any one of [1] to

[14] .

[18] A circuit board comprising an insulating layer made of a cured product of the resin composition according to any one of [1] to

[14] .

[19] A semiconductor device comprising the circuit board according to

[18] . Effect of the Invention

[0008] According to the present invention, it is possible to provide a resin composition capable of giving a cured product having excellent resin flatness and exhibiting good dielectric properties and peel strength; a resin sheet containing the resin composition; a circuit board having an insulating layer formed using the resin composition, and a semiconductor device. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0009] <Terminology explanation> As used herein, the term "optionally substituted" in reference to a compound or group means both the case where the hydrogen atoms of the compound or group are not substituted with substituents, and the case where some or all of the hydrogen atoms of the compound or group are substituted with substituents.

[0010] In this specification, unless otherwise specified, the term "substituent" means a halogen atom, an alkyl group, an alkenyl group, a cycloalkyl group, an alkoxy group, a cycloalkyloxy group, an aryl group, an aryloxy group, an arylalkyl group, an arylalkoxy group, a monovalent heterocyclic group, an alkylidene group, an amino group, a silyl group, a carboxy group, a sulfo group, a cyano group, a nitro group, a hydroxy group, a mercapto group, and an oxo group.

[0011] Examples of halogen atoms used as a substituent include a fluorine atom, a chlorine atom, a bromine atom, and an iodine atom. The alkyl group used as a substituent may be either linear or branched. The number of carbon atoms in the alkyl group is preferably 1 to 12, more preferably 1 to 6, and even more preferably 1 to 3. The alkenyl group used as a substituent may be either linear or branched. The number of carbon atoms in the alkenyl group is preferably 2 to 12, more preferably 2 to 6, and even more preferably 2 or 3. The number of carbon atoms in the cycloalkyl group used as a substituent is preferably 3 to 12, more preferably 3 to 6. The alkoxy group used as a substituent may be either linear or branched. The number of carbon atoms in the alkoxy group is preferably 1 to 12, more preferably 1 to 6. The number of carbon atoms in the cycloalkyloxy group used as a substituent is preferably 3 to 12, more preferably 3 to 6. The aryl group used as a substituent is a group obtained by removing one hydrogen atom on the aromatic ring from an aromatic hydrocarbon. The number of carbon atoms in the aryl group used as a substituent is preferably 6 to 14, more preferably 6 to 10. The number of carbon atoms of the aryloxy group used as a substituent is preferably 6 to 14, more preferably 6 to 10. The number of carbon atoms of the arylalkyl group used as a substituent is preferably 7 to 15, more preferably 7 to 11. The number of carbon atoms of the arylalkoxy group used as a substituent is preferably 7 to 15, more preferably 7 to 11. The monovalent heterocyclic group used as a substituent refers to a group in which one hydrogen atom is removed from the heterocycle of a heterocyclic compound. The number of carbon atoms of the monovalent heterocyclic group is preferably 3 to 15, more preferably 3 to 9. The alkylidene group used as a substituent refers to a group in which two hydrogen atoms are removed from the same carbon atom of an alkane. The number of carbon atoms of the alkylidene group is preferably 1 to 12, more preferably 1 to 6, and even more preferably 1 to 3. The above-mentioned substituent may further have a substituent (hereinafter sometimes referred to as a "secondary substituent"). Unless otherwise specified, the same one as the above-mentioned substituent may be used as the secondary substituent.

[0012] In this specification, the term "aromatic ring" means a ring that follows the Huckel rule, in which the number of electrons in the π-electron system on the ring is 4p+2 (p is a natural number), and includes monocyclic aromatic rings and polycyclic aromatic rings such as fused polycyclic aromatic rings in which two or more monocyclic aromatic rings are fused. The aromatic ring may be an aromatic carbocycle having only carbon atoms as ring-constituting atoms, or an aromatic heterocycle having heteroatoms such as oxygen atoms, nitrogen atoms, and sulfur atoms in addition to carbon atoms as ring-constituting atoms. In this specification, the number of carbon atoms in the aromatic ring is preferably 3 or more, more preferably 4 or more or 5 or more, and even more preferably 6 or more, unless otherwise specified, and the upper limit is preferably 24 or less, more preferably 18 or less or 14 or less, and even more preferably 10 or less. The number of carbon atoms of the substituent is not included in the number of carbon atoms. Hereinafter, a structure containing an aromatic ring is also referred to as an "aromatic ring structure", and a skeleton containing an aromatic ring is also referred to as an "aromatic ring skeleton".

[0013] In the present specification, the term "aliphatic ring" means a ring other than an aromatic ring. The aliphatic ring may have a double bond in a part of the ring. The aliphatic ring may be a monocyclic aliphatic ring or a bridged aliphatic ring such as a bicyclo ring or a tricyclo ring. The aliphatic ring may be an aliphatic carbon ring having only carbon atoms as ring-constituting atoms, or an aliphatic heterocycle having heteroatoms in addition to carbon atoms as ring-constituting atoms. In the present specification, the number of carbon atoms in the aliphatic ring is preferably 3 or more, more preferably 4 or more or 5 or more, and even more preferably 6 or more, unless otherwise specified, and the upper limit is preferably 24 or less, more preferably 18 or less or 14 or less, and even more preferably 10 or less. Hereinafter, a structure containing an aliphatic ring is also referred to as an "alicyclic structure".

[0014] The present invention will be described in detail below with reference to preferred embodiments. However, the present invention is not limited to the following embodiments and examples, and can be modified and implemented as desired without departing from the scope of the claims of the present invention and their equivalents.

[0015] [Resin composition] The resin composition of the present invention is a resin composition containing a radical polymerizable resin A having a ring structure in the main skeleton, and di-t-amyl peroxide. In the present invention, by using the radical polymerizable resin A in combination with di-t-amyl peroxide, it is possible to obtain a cured product having excellent resin flatness, good dielectric properties, and peel strength.

[0016] The resin composition may further contain optional components in addition to the radical polymerizable resin A and di-t-amyl peroxide. Examples of the optional components include inorganic fillers, thermoplastic resins, thermosetting resins, curing accelerators, and other additives. Each component contained in the resin composition will be described in detail below.

[0017] <Radical polymerizable resin A> The resin composition of the present invention contains a radical polymerizable resin A. The radical polymerizable resin A is a compound containing a ring structure in the main skeleton and having a radical polymerizable unsaturated group. By including the radical polymerizable resin A, it becomes possible to obtain a cured product having excellent surface flatness, good dielectric properties, peel strength, and excellent heat resistance. The radical polymerizable resin A may be used alone, but from the viewpoint of being able to enjoy the effects of the present invention more effectively in combination with di-t-amyl peroxide, it is preferable to use two or more kinds in combination.

[0018] The radical polymerizable resin A contains a ring structure in the main skeleton. The ring structure may be either an aromatic ring structure or an alicyclic structure, and the aromatic ring and the aliphatic ring contained in these ring structures are as described above. From the viewpoint of being able to enjoy the effects of the present invention more effectively in combination with di-t-amyl peroxide, it is preferable that the radical polymerizable resin A contains a radical polymerizable resin containing an aromatic ring structure in the main skeleton.

[0019] The radical polymerizable resin A contains a radical polymerizable unsaturated group that exhibits radical polymerization activity by the action of a free radical. Examples of the radical polymerizable unsaturated group include one or more selected from a maleimide group, a vinyl group, a propenyl group (1-propenyl group), an allyl group (2-propenyl group), a styryl group, a vinylphenyl group, an acryloyl group, a methacryloyl group, a fumaroyl group, and a maleoyl group. Among them, from the viewpoint of being able to enjoy the effects of the present invention more in combination with di-t-amyl peroxide, and from the viewpoint of providing an insulating layer with excellent resin flatness, the radical polymerizable unsaturated group is preferably one or more selected from a maleimide group, a vinyl group, an allyl group, a styryl group, a vinylphenyl group, an acryloyl group, and a methacryloyl group. Particularly from the viewpoint of easily enjoying the effects of the present invention, the radical polymerizable resin A is preferably any one of a maleimide resin, a terminal double bond-modified polyphenylene ether resin, an allyl resin, a propenyl resin, and a (meth)acrylic resin.

[0020] -Maleimide resin- The maleimide resin that can be contained in the resin composition of the present invention has a maleimide group and a ring structure in the main skeleton. The maleimide resin may be used alone or in combination of two or more kinds.

[0021] Such maleimide resins include: (A1) a maleimide resin containing an aliphatic group having 5 or more carbon atoms directly bonded to a nitrogen atom of the maleimide; (A2) a maleimide resin containing a trimethylindane skeleton, and (A3) a maleimide resin having an aromatic ring directly bonded to a nitrogen atom of the maleimide; It is preferable that the compound is one or more selected from the following:

[0022] The term "directly" as used herein means that, in the case of component (A1), there are no other groups between the nitrogen atom of the maleimide and the aliphatic group having 5 or more carbon atoms, and in the case of component (A3), there are no other groups between the nitrogen atom of the maleimide and the aromatic ring.

[0023] Regardless of whether the maleimide resin is component (A1), component (A2), or component (A3), it is preferable that the maleimide resin has two or more maleimide groups (2,5-dihydro-2,5-dioxo-1H-pyrrol-1-yl groups) in one molecule.

[0024] Hereinafter, the components (A1), (A2), and (A3), which are suitable embodiments of the maleimide resin, will be explained. In the following, the term "substituent" is as defined in <Explanation of Terms> above.

[0025] <Component (A1)> The component (A1) is a maleimide resin containing an aliphatic group having 5 or more carbon atoms directly bonded to a nitrogen atom of the maleimide. Such a maleimide resin can be obtained, for example, by subjecting a component containing an aliphatic amine compound (such as a dimer diamine compound), maleic anhydride, and, as necessary, tetracarboxylic dianhydride to an imidization reaction.

[0026] The component (A1) includes a compound represented by the following formula (A1-1).

[0027] [ka]

[0028] In formula (A1-1), A 1 represents an aliphatic group having 5 or more carbon atoms which may have a substituent, L 1 represents a single bond or a divalent linking group, nB1 represents an integer from 0 to 20. 1 When there are multiple, they may be the same or different, and L 1 When there are multiple, they may be the same or different.

[0029] A 1The number of carbon atoms in the aliphatic group represented by the formula (I) is 5 or more, and preferably 10 or more, 15 or more, or 20 or more. The upper limit of the number of carbon atoms is not particularly limited, and may be, for example, 100 or less, 80 or less, 60 or less, or 50 or less. The number of carbon atoms does not include the number of carbon atoms of the substituent.

[0030] In one embodiment, A 1 is a divalent group represented by the following formula (A1-2).

[0031] [ka]

[0032] In formula (A1-2), A 11 represents a single bond, an alkylene group, or an alkenylene group (preferably an alkylene group or an alkenylene group), Ring Z 1 represents a non-aromatic ring optionally having a group selected from an alkyl group and an alkenyl group (preferably a cycloalkane ring or cycloalkene ring optionally having a group selected from an alkyl group and an alkenyl group), nB11 represents an integer of 0 to 3 (preferably 0 or 1, more preferably 1); * indicates the binding site. 11 Or Z 1 Each of A may independently have a substituent. 11 When there are multiple rings, they may be the same or different. 1 When there are multiple, they may be the same or different.

[0033] L 1 Examples of the divalent linking group represented by the formula (A1-3) include divalent organic groups (preferably divalent ring-containing organic groups (e.g., aromatic rings or non-aromatic rings)) consisting of two or more (e.g., 2 to 3000, 2 to 1000, 2 to 100, or 2 to 50) skeletal atoms selected from carbon atoms, oxygen atoms, nitrogen atoms, and sulfur atoms, and among these, divalent groups represented by the formula (A1-3) below are preferred.

[0034] [ka]

[0035] In formula (A1-3), A 12 represents a single bond or a divalent group consisting of one or more (e.g., 1 to 3000, 1 to 1000, 1 to 100, or 1 to 50) skeletal atoms selected from carbon atoms, oxygen atoms, nitrogen atoms, and sulfur atoms, R B1 and R B2 each independently represents a substituent, nB12 represents 0 or 1; nB13 and nB14 each independently represent an integer of 0 to 3 (preferably 0 or 1), * indicates the binding site. B1 When there are multiple, they may be the same or different, and R B2 When there are multiple, they may be the same or different.

[0036] When nB12 is 0, the divalent group represented by formula (A1-3) is a divalent group having a structure represented by the following formula (A1-4): B1 , nB13 and * are as explained in formula (A1-3).

[0037] [ka]

[0038] In the embodiment in which nB12 in formula (A1-3) is 1, A 12 The divalent group represented by the following formula (A1-5) is preferable.

[0039] [ka]

[0040] In formula (A1-5), Y 1represents a single bond, an alkylene group, an alkenylene group, -O-, -CO-, -S-, -SO-, -SO2-, -CONH-, -NHCO-, -COO-, or -OCO-; Ring Z 2 represents an optionally substituted non-aromatic ring or an optionally substituted aromatic ring, nB15 represents an integer of 0 to 5 (preferably 0 to 3), * indicates the binding site. 1 Or Z 2 Each of Y may independently have a substituent. 1 When there are multiple rings, they may be the same or different. 2 When there are multiple, they may be the same or different.

[0041] A 12 Specific examples of the divalent group represented by the formula (I) include, but are not limited to, -CH-, -CH(CH)-, -CH(CHCH)-, -C(CH)-, -C(CH)(CHCH)-, -C(CHCH)-, -O-, -CO-, -S-, -SO-, and -SO-, as well as divalent organic groups represented by the formula (I) below.

[0042] [ka]

[0043] The weight average molecular weight (Mw) of the component (A1) is not particularly limited, but is preferably 150 to 50,000, more preferably 300 to 20,000, and more specifically, in an embodiment in which nB1 in formula (A1-1) is an integer of 1 or more, it is preferably 500 to 50,000, more preferably 1,000 to 20,000, and in an embodiment in which nB1 is 0, it is preferably 150 to 5,000, more preferably 300 to 1,000. The Mw of the component (A1) can be measured as a polystyrene-equivalent value by gel permeation chromatography (GPC).

[0044] Furthermore, with regard to the component (A1), the functional group equivalent (active group equivalent) of the maleimide group is preferably 50 to 20,000 g / eq, more preferably 100 to 20,000 g / eq.; more specifically, in an embodiment in which nB1 in formula (E1-1) is an integer of 1 or greater, it is preferably 300 g / eq. to 20,000 g / eq., more preferably 500 g / eq. to 10,000 g / eq.; and in an embodiment in which nB1 is 0, it is preferably 50 g / eq. to 2,000 g / eq., more preferably 100 g / eq. to 1,000 g / eq., even more preferably 200 g / eq. to 600 g / eq., and particularly preferably 300 g / eq. to 400 g / eq.

[0045] From the viewpoint of providing a cured product of the resin composition that has an excellent surface flatness, good dielectric properties and peel strength, and also has excellent heat resistance, it is preferable that the component (A1) contains a maleimide resin having any of a structure represented by the following formula (A1-6), a structure represented by the following formula (A1-7), or a structure represented by the following formula (A1-8).

[0046] [ka]

[0047] In formula (A1-6), A 11 and ring Z 1 is as explained above, and A 11 -Ring Z 1 -A 11 The number of carbon atoms per block is preferably 20 to 100 (more preferably 30 to 60 or 30 to 50), and it is particularly preferably a so-called dimer acid skeleton (C36 skeleton; C36 alkylene skeleton derived from dimer diamine). nB16 represents an integer of 1 to 10.

[0048] [ka] In formula (A1-7), A 11 , Y 1 , ring Z 1 , ring Z 2and nB15 are as described above, and A 11 -Ring Z 1 -A 11 The number of carbon atoms per block is preferably 20 to 100 (more preferably 30 to 60 or 30 to 50), and it is particularly preferably a so-called dimer acid skeleton (C36 skeleton; C36 alkylene skeleton derived from dimer diamine). In addition, the block consisting of nB15+1 Y1 and nB15 rings Z2 is preferably a divalent group A 12 Among them, a divalent group containing an oxygen atom is preferable. nB17 represents an integer of 1 to 10.

[0049] [ka]

[0050] In formula (A1-8), A 11 and ring Z 1 is as explained above, and A 11 -Ring Z 1 -A 11 The number of carbon atoms per block is preferably 20 to 100 (more preferably 30 to 60 or 30 to 50), and it is particularly preferably a so-called dimer acid skeleton (C36 skeleton; C36 alkylene skeleton derived from dimer diamine). nB11 represents an integer of 0 to 10.

[0051] Commercially available maleimide resins having a structure represented by formula (A1-6) include, for example, "BMI-3000J" and "BMI-5000" manufactured by Designer Molecules Inc. Commercially available maleimide resins having a structure represented by formula (A1-7) include, for example, "BMI-1400", "BMI-1500", and "BMI-1700" manufactured by Designer Molecules Inc. Commercially available maleimide resins having a structure represented by formula (A1-8) include, for example, "BMI-689" manufactured by Designer Molecules Inc.

[0052] <(A2) component> The component (A2) is a maleimide resin containing a trimethylindane skeleton, which is represented by the following formula (A2-1).

[0053] [ka]

[0054] The benzene ring in the trimethylindane skeleton may have a substituent. When the benzene ring in the trimethylindane skeleton has a substituent, the number of the substituent may be 1 or 2 or more. The upper limit of the number of the substituents that the benzene ring in the trimethylindane skeleton has is usually 3 or less. When the number of the substituents is 2 or more, they may be the same or different from each other. Among them, it is preferable that the benzene ring in the trimethylindane skeleton does not have a substituent.

[0055] The number of trimethylindane structures contained in one molecule of the component (A2) may be 1, or may be equal to or greater than 2. The upper limit can be, for example, 10 or less, 8 or less, 7 or less, or 6 or less.

[0056] The component (A2) preferably further contains an aromatic ring skeleton in addition to the above-mentioned trimethylindane skeleton. The aromatic ring skeleton may be either a carbon ring skeleton or a heterocyclic skeleton, but a carbon ring skeleton is more preferable. The number of ring carbon atoms of the aromatic ring skeleton is preferably 3 to 20, more preferably 4 to 16, 5 to 14, or 6 to 10. Examples of the aromatic ring skeleton include a benzene ring skeleton, a naphthalene ring skeleton, and an anthracene ring skeleton. The number of aromatic ring skeletons contained in one molecule of the component (A2) is preferably 1 or more, more preferably 2 or more, and preferably 6 or less, more preferably 4 or less, and even more preferably 3 or less. When the component (A2) contains two or more aromatic ring skeletons in addition to the trimethylindane skeleton, the aromatic ring skeletons may be the same or different from each other.

[0057] The aromatic ring skeleton may have a substituent. When the aromatic ring skeleton has a substituent, the number of the substituent may be 1 or 2 or more. The upper limit of the number of the substituent that the aromatic ring skeleton has is usually 4 or less. When the number of the substituents is 2 or more, they may be the same or different from each other.

[0058] The (A2) component preferably contains a divalent aliphatic hydrocarbon group in addition to the trimethylindane skeleton. In particular, when the (A2) component contains an aromatic ring skeleton in addition to the benzene ring in the trimethylindane skeleton, the (A2) component preferably contains a divalent aliphatic hydrocarbon group. In this case, the divalent aliphatic hydrocarbon group preferably connects the benzene ring and the aromatic ring skeleton in the trimethylindane skeleton. In addition, the divalent aliphatic hydrocarbon group preferably connects the aromatic ring skeletons together.

[0059] The number of carbon atoms of the divalent aliphatic hydrocarbon group is preferably 1 or more, preferably 12 or less, more preferably 8 or less, and even more preferably 5 or less. The divalent aliphatic hydrocarbon group may be either a divalent saturated hydrocarbon group or a divalent unsaturated hydrocarbon group, but is preferably a divalent saturated hydrocarbon group, and more preferably an alkylene group. Examples of the divalent aliphatic hydrocarbon group include linear alkylene groups such as methylene, ethylene, trimethylene, tetramethylene, pentamethylene, and hexamethylene; and branched alkylene groups such as ethylidene (-CH(CH3)-), propylidene (-CH(CH2CH3)-), isopropylidene (-C(CH3)2-), ethylmethylmethylene (-C(CH3)(CH2CH3)-), and diethylmethylene (-C(CH2CH3)2-). When the component (A2) contains two or more divalent aliphatic hydrocarbon groups in addition to the trimethylindane skeleton, those divalent aliphatic hydrocarbon groups may be the same or different.

[0060] From the viewpoint of providing a cured product of the resin composition with excellent surface flatness, good dielectric properties, peel strength, and excellent heat resistance, it is preferable that the (A2) component contains a structure represented by the following formula (A2-2): The entire (A2) component may have a structure represented by formula (A2-2), or only a part of the (A2) component may have a structure represented by formula (A2-2).

[0061] [ka]

[0062] In formula (A2-2), Ar a1 represents a divalent aromatic ring group which may have a substituent, R a1 and R a2 each independently represents a substituent, R a3 represents a divalent aliphatic hydrocarbon group, n a1 represents a positive integer, n a2 each independently represents an integer of 0 to 4, n a3 R each independently represents an integer of 0 to 3. a1 When there are multiple, they may be the same or different, and R a2 If there are multiple R a3 may be the same or different from each other.

[0063] Ar a1represents a divalent aromatic ring group which may have a substituent. The number of carbon atoms in the divalent aromatic ring group is preferably 6 or more, and preferably 20 or less, more preferably 16 or less, 14 or less, or 10 or less. Examples of the divalent aromatic ring group include a phenylene group and a naphthylene group. Examples of the substituent that the divalent aromatic ring group may have include the above-mentioned substituents, and among them, an alkyl group having 1 to 10 carbon atoms, an alkyloxy group having 1 to 10 carbon atoms, an alkylthio group having 1 to 10 carbon atoms, an aryl group having 6 to 10 carbon atoms, an aryloxy group having 6 to 10 carbon atoms, an arylthio group having 6 to 10 carbon atoms, a cycloalkyl group having 3 to 10 carbon atoms, a halogen atom, a hydroxyl group, and a mercapto group are preferred. The hydrogen atom of each substituent may be further substituted with a halogen atom. When the divalent aromatic ring group has a substituent, the number of the substituent is preferably 1 to 4. When the divalent aromatic ring group has two or more substituents, the two or more substituents may be the same or different. a1 is preferably a divalent aromatic ring group having no substituent.

[0064] R a1 R represents a substituent. a1 Examples of the substituent represented by the formula (I) include the aforementioned substituents, and among them, an alkyl group having 1 to 10 carbon atoms, an alkyloxy group having 1 to 10 carbon atoms, an alkylthio group having 1 to 10 carbon atoms, an aryl group having 6 to 10 carbon atoms, an aryloxy group having 6 to 10 carbon atoms, an arylthio group having 6 to 10 carbon atoms, a cycloalkyl group having 3 to 10 carbon atoms, a halogen atom, a nitro group, a hydroxyl group, and a mercapto group are preferred. The hydrogen atom of each of the substituents may be further substituted with a halogen atom.

[0065] Among them, R a1 is more preferably one or more groups selected from the group consisting of an alkyl group having 1 to 4 carbon atoms, a cycloalkyl group having 3 to 6 carbon atoms, and an aryl group having 6 to 10 carbon atoms, and is further preferably an alkyl group having 1 to 4 carbon atoms.

[0066] Ra2 R represents a substituent. a2 Examples of the substituent represented by the formula (I) include the aforementioned substituents, and among them, an alkyl group having 1 to 10 carbon atoms, an alkyloxy group having 1 to 10 carbon atoms, an alkylthio group having 1 to 10 carbon atoms, an aryl group having 6 to 10 carbon atoms, an aryloxy group having 6 to 10 carbon atoms, an arylthio group having 6 to 10 carbon atoms, a cycloalkyl group having 3 to 10 carbon atoms, a halogen atom, a hydroxyl group, and a mercapto group are preferred. The hydrogen atom of each of the substituents may be further substituted with a halogen atom.

[0067] Among them, R a2 is more preferably one or more groups selected from the group consisting of an alkyl group having 1 to 4 carbon atoms, a cycloalkyl group having 3 to 6 carbon atoms, and an aryl group having 6 to 10 carbon atoms.

[0068] R a3 represents a divalent aliphatic hydrocarbon group. The preferred range of the divalent aliphatic hydrocarbon group is as described above.

[0069] n a1 represents a positive integer. a1 is preferably 1 or more, and preferably 10 or less, more preferably 8 or less.

[0070] n a2 Each independently represents an integer of 0 to 4. a2 is preferably 2 or 3, more preferably 2. a2 may be different from each other, but are preferably the same. a2 If is 2 or more, multiple R a1 may be the same or different from each other.

[0071] n a3 represents an integer of 0 to 3. a3 When there are a plurality of n, they may be different from each other, but are preferably the same as each other. a3 is preferably 0.

[0072] From the viewpoint of providing a cured product of the resin composition with excellent surface flatness, good dielectric properties, peel strength, and excellent heat resistance, it is further preferable that the (A2) component contains a structure represented by the following formula (A2-3): The entire (A2) component may have a structure represented by formula (A2-3), or only a part of the (A2) component may have a structure represented by formula (A2-3).

[0073] [ka]

[0074] In formula (A2-3), R a1 , R a2 , n a1 , n a2 and n a3 is as explained in formula (A2-2).

[0075] The component (A2) may further contain a structure represented by the following formula (A2-4).

[0076] [ka]

[0077] In formula (A2-4), R a1 , R a2 , n a2 and n a3 is as explained in formula (A2-2). c1 is the number of repeating units and represents an integer of 1 to 20. * represents a bond.

[0078] For example, the component (A2) is a compound represented by the formula (A2-2): a2 is 3 or less, and R is present at two or more of the ortho and para positions relative to the maleimide group bonding position of the benzene ring to which the maleimide group is bonded. a1 When is not bonded, the structure represented by formula (A2-2) may include a structure represented by formula (A2-4) in combination with the structure represented by formula (A2-2).

[0079] Furthermore, for example, the component (A2) is a compound represented by the formula (A2-3), a2 is 3 or less, and R is present at two or more of the ortho and para positions relative to the maleimide group bonding position of the benzene ring to which the maleimide group is bonded. a1 When is not bonded, the structure represented by formula (A2-3) may include a structure represented by formula (A2-4) in combination with the structure represented by formula (A2-4).

[0080] The method for producing the component (A2) is not particularly limited, and may be produced, for example, by the method described in the Japan Institute of Invention and Innovation Disclosure Technical Bulletin No. 2020-500211. According to the production method described in this Japan Institute of Invention and Innovation Disclosure Technical Bulletin No. 2020-500211, a maleimide resin having a distribution in the number of repeating units of the trimethylindane skeleton can be obtained. The maleimide resin obtained by this method contains a structure represented by the following formula (A2-5). Therefore, the maleimide resin may contain a maleimide resin containing a structure represented by formula (A2-5).

[0081] [ka]

[0082] In formula (A2-5), R 1 , R 2 , n2 and n3 are each R in formula (A2-2). a1 , R a2 , n a2 and n a3 The preferred types and ranges are also the same as those in the above. n1 represents the average number of repeating units of 0.95 to 10.0.

[0083] In formula (A2-5), n1 represents the average number of repeating units, and its range is 0.95 to 10.0. According to the manufacturing method described in the Japan Institute of Invention and Innovation Disclosure Technical Bulletin No. 2020-500211, a group of maleimide resins containing a structure represented by formula (A2-5) can be obtained. As can be seen from the fact that the average number of repeating units n1 in formula (A2-5) can be smaller than 1.00, the maleimide resin containing the structure represented by formula (A2-5) thus obtained can contain a maleimide resin having a trimethylindane skeleton repeating unit number of 0. Therefore, the maleimide resin containing the structure represented by formula (A2-5) is purified to remove the maleimide resin having a trimethylindane skeleton repeating unit number of 0 to obtain the (A2) component, and the resin composition may contain only the obtained (A2) component, or it is preferable that the resin composition contains a maleimide resin containing a structure represented by formula (A2-5) without removing the maleimide resin having a trimethylindane skeleton repeating unit number of 0.

[0084] In formula (A2-5), the average number of repeating units n1 is preferably 0.95 or more, more preferably 0.98 or more, even more preferably 1.0 or more, particularly preferably 1.1 or more, and is preferably 10.0 or less, more preferably 8.0 or less, even more preferably 7.0 or less, particularly preferably 6.0 or less. When the average number of repeating units n1 is within this range, the effects of the present invention can be significantly obtained.

[0085] Among others, specific examples of the structure of the component (A2) include the following:

[0086] [ka]

[0087] The maleimide resin containing the structure represented by formula (A2-5) may further contain the structure represented by formula (A2-4) above. For example, the maleimide resin containing the structure represented by formula (A2-5) may be a maleimide resin containing a structure represented by formula (A2-5) in which n2 is 3 or less and R is present at two or more of the ortho and para positions relative to the maleimide group bonding position of the benzene ring to which the maleimide group is bonded.1 When is not bonded, the structure represented by formula (A2-5) may include a structure represented by formula (A2-4) in combination.

[0088] The maleimide resin containing the structure represented by formula (A2-5) preferably has a molecular weight distribution Mw / Mn calculated by gel permeation chromatography (GPC) measurement in a specific range. Specifically, the molecular weight distribution Mw / Mn of the maleimide resin containing the structure represented by formula (A2-5) is preferably 1.0 to 4.0, more preferably 1.1 to 3.8, even more preferably 1.2 to 3.6, and particularly preferably 1.3 to 3.4.

[0089] With respect to the component (A2), the functional group equivalent (active group equivalent) of the maleimide group is preferably 50 g / eq. or more, more preferably 100 g / eq. or more, even more preferably 200 g / eq. or more, and is preferably 2000 g / eq. or less, more preferably 1000 g / eq. or less, even more preferably 800 g / eq. or less.

[0090] <(A3) component> The component (A3) is a maleimide resin having an aromatic ring directly bonded to a nitrogen atom of the maleimide. Such a maleimide resin can be obtained, for example, by subjecting a component containing an aromatic amine compound (such as an aromatic diamine compound) and maleic anhydride to an imidization reaction.

[0091] In one embodiment, the component (A3) includes a compound represented by the following formula (A3-1):

[0092] [ka]

[0093] In formula (A3-1), Ring Ar 1 represents an aromatic ring which may have a substituent, L 2 represents a single bond or a divalent linking group, nB2 represents an integer of 1 to 100. 1 may be the same or different, L 2 When there are multiple, they may be the same or different.

[0094] Ring Ar 1 The aromatic ring represented by the formula (I) may be either a carbocyclic ring or a heterocyclic ring, but is preferably a carbocyclic ring. 1 The number of carbon atoms in the aromatic ring represented by the following formula is preferably 3 to 20, and more preferably 5 to 14 or 6 to 10. The number of carbon atoms does not include the number of carbon atoms of the substituent.

[0095] L 2 The divalent linking group represented by the formula (A1-3) is not particularly limited as long as it is a divalent group consisting of one or more (for example, 1 to 3000, 1 to 1000, 1 to 100, or 1 to 50) skeletal atoms selected from carbon atoms, oxygen atoms, nitrogen atoms, and sulfur atoms. For example, the divalent group represented by the formula (A1-5) and the above-mentioned A 12 Examples of the divalent group include the divalent group shown in

[0096] Among them, the ring Ar 1 is preferably an aromatic carbocyclic ring having 6 to 10 carbon atoms which may have a substituent (more preferably a benzene ring which may have a substituent), and L 2 (L 2 If there are multiple L, at least one 2 is preferably a divalent group having a biphenyl skeleton. Thus, in one embodiment, the component (A3) has a biphenyl skeleton.

[0097] In the (A3) component, the nitrogen atom of the maleimide is directly bonded to the aromatic ring. The bonding position of the maleimide to the aromatic ring is the same as that of the L bonded to the aromatic ring. 2 For example, when the aromatic ring is a benzene ring, the bonding position of the maleimide to the benzene ring may be any position based on the position of L bonded to the benzene ring. 2Based on this standard, the bond may be at any of the ortho, meta, and para positions, but it is preferred that the bond be at the para position in order to obtain the effects of the present invention more effectively.

[0098] In a preferred embodiment, the component (A3) includes a compound represented by the following formula (A3-2):

[0099] [ka]

[0100] In formula (A3-2), R B3 , R B4 , R B5 and R B6 each independently represents a substituent, nB21 represents an integer from 1 to 100, nB22 and nB23 each independently represent an integer of 1 to 10; nB24 and nB25 each independently represent an integer of 0 to 3; nB26 and nB27 each independently represent an integer of 0 to 4. B3 When there are multiple, they may be the same or different, which means that R B4 , R B5 and R B6 The same applies to.

[0101] nB21 is preferably 1-50, more preferably 1-20, and further preferably 1-5.

[0102] nB22 and nB23 each independently represent preferably 1 to 6, more preferably 1 to 3, and further preferably 1 or 2.

[0103] nB24 and nB25 are each independently preferably an integer of 0 to 2, more preferably 0 or 1. When nB24 and nB25 are 1 or more, R B3 and R B4 It is preferable that each of the substituents represented by the following formula (I) is independently an alkyl group or an aryl group.

[0104] nB26 and nB27 are each independently preferably an integer of 0 to 2, more preferably 0 or 1. When nB26 and nB27 are 1 or more, R B5 and R B6 It is preferable that each of the substituents represented by the following formula (I) is independently an alkyl group or an aryl group.

[0105] Of these, nB26 and nB27 are preferably 0. Therefore, in a preferred embodiment, the component (A3) includes a compound represented by the following formula (A3-3).

[0106] [ka]

[0107] In formula (A3-3), R B3 , R B4 , nB21, nB22, nB23, nB24, and nB25 are as explained in formula (A2-2).

[0108] When the component (A3) has a molecular weight distribution, the weight average molecular weight (Mw) is at least 500, and preferably at least 550. There are no particular limitations on the upper limit of Mw, but it is preferably at most 5000, and more preferably at most 2500. The Mw of the component (A2) can be measured as a polystyrene-equivalent value by gel permeation chromatography (GPC).

[0109] Furthermore, for the component (A3), the functional group equivalent (active group equivalent) of the maleimide group is preferably 50 g / eq. to 2000 g / eq., more preferably 100 g / eq. to 1000 g / eq., even more preferably 150 g / eq. to 500 g / eq., and particularly preferably 200 g / eq. to 300 g / eq.

[0110] From the viewpoint of providing a cured product of the resin composition that has excellent surface flatness, excellent dielectric properties, excellent peel strength, and also excellent heat resistance, it is preferable that the component (A2) contains a maleimide resin having a structure represented by the following formula (A3-4).

[0111] [ka]

[0112] In the formula (A3-4), nB21 is as explained above.

[0113] Commercially available maleimide resins having the structure represented by formula (A3-4) include, for example, "MIR-3000-70MT" and "MIR-5000-60T" manufactured by Nippon Kayaku Co., Ltd. As the component (A3), "BMI-4000" manufactured by Daiwa Kasei Co., Ltd. and "BMI-80" manufactured by Keiai Kasei Co., Ltd. may also be used as the compound represented by formula (A3-1).

[0114] -Terminal double bond modified polyphenylene ether resin- The terminal double bond-modified polyphenylene ether resin contains a polyphenylene ether skeleton including a plurality of phenylene ether structural units represented by the following formula (A4-1).

[0115] [ka] (In formula (A4-1), R each independently represents a halogen atom, an optionally substituted alkyl group, an optionally substituted alkoxy group, an optionally substituted aryl group, an optionally substituted amino group, a nitro group, or a carboxy group; m represents an integer of 0 to 4.

[0116] The alkyl group or alkoxy group in R may be either linear or branched, and has preferably 1 to 10 carbon atoms, more preferably 1 to 6, and further preferably 1 to 4 or 1 to 3. The number of carbon atoms does not include the number of carbon atoms of the substituent.

[0117] The number of carbon atoms in the aryl group for R is preferably 6 to 14, and more preferably 6 to 10. The number of carbon atoms does not include the number of carbon atoms of the substituent.

[0118] The substituent that the monovalent group represented by R may have is as described above, and among them, it is preferably one or more selected from a halogen atom, an alkyl group, an alkoxy group, and an aryl group, more preferably one or more selected from a halogen atom, an alkyl group, and an aryl group, and further preferably one or more selected from a fluorine atom, an alkyl group having 1 to 6 carbon atoms, and an aryl group having 6 to 10 carbon atoms.

[0119] In formula (1), m represents an integer of 0 to 4, preferably an integer of 0 to 3, and more preferably an integer of 1 to 3.

[0120] From the viewpoint of obtaining good dielectric properties, the polyphenylene ether skeleton is preferably an oligophenylene ether skeleton containing a plurality of one or more units selected from the group consisting of 2,6-disubstituted-1,4-phenylene ether units, 2,5-disubstituted-1,4-phenylene ether units, and 2,3,6-trisubstituted-1,4-phenylene ether units, and among these, an oligophenylene ether skeleton containing a plurality of 2,6-disubstituted-1,4-phenylene ether units is preferred (wherein the substituents at the 2,6-positions, the substituents at the 2,5-positions, and the substituents at the 2,3,6-positions correspond to R in formula (A4-1)).

[0121] Specific examples of suitable polyphenylene ether backbones include poly(2,6-disubstituted-1,4-phenylene ether) backbones such as poly(2,6-dialkyl-1,4-phenylene ether) backbones, poly(2-alkyl-6-aryl-1,4-phenylene ether) backbones, poly(2,6-diaryl-1,4-phenylene ether) backbones, and poly(2,6-dihalo-1,4-phenylene ether) backbones; 2,6-disubstituted phenols and other phenolic compounds (e.g., 2,5-dialkyl phenols); and 2,3,6-trisubstituted phenols such as 2,5-diphenylphenol, 2-alkyl-5-arylphenol, and 2,5-diarylphenol; and 2,3,6-trisubstituted phenols such as 2,3,6-trialkylphenol and 2,3,6-trihalophenol; and polyphenylene ether skeletons containing a plurality of 2,6-disubstituted-1,4-phenylene ether units, such as a coupling reaction product of 2,6-disubstituted phenol and a biphenol compound or a bisphenol compound.

[0122] From the viewpoint of providing a cured product exhibiting good dielectric properties, the polyphenylene ether skeleton preferably contains a structure represented by the following formula (A4-2).

[0123] [ka] In formula (A4-2), R each independently represents a halogen atom, an optionally substituted alkyl group, an optionally substituted alkoxy group, an optionally substituted aryl group, an optionally substituted amino group, a nitro group, or a carboxy group; m represents an integer of 0 to 4. L represents a divalent linking group. n1 and n2 each independently represent an integer of 1 to 100. Each X independently represents (i) a (meth)acryloyl group, or (ii) a divalent group represented by the following formula (A4-3).

[0124] [ka] In formula (A4-3), R has the same meaning as in formula (A4-1). A represents an alkylene group which may have a substituent. Y represents an alkenyl group or a (meth)acryloyloxy group; m1 represents an integer of 0 to 4.

[0125] In formula (A4-2), L represents a divalent linking group. Examples of the divalent linking group include a single bond, an alkylene group which may have a substituent, an alkenylene group which may have a substituent, an arylene group which may have a substituent, an alkylarylene group which may have a substituent, a heteroarylene group which may have a substituent, -O-, -NH-, -NRx-, -CO-, -CS-, -SO-, -SO2-, -C(=O)O-, -NHC(=O)-, -NC(=O)N-, -NHC(=O)O-, -C(=O)-, -S-, and a divalent group formed by combining a plurality of these. Here, Rx represents a hydrocarbon group having 1 to 12 carbon atoms.

[0126] Among these, from the viewpoint of obtaining the effects of the present invention more effectively, the divalent linking group represented by L is preferably a single bond, an alkylene group which may have a substituent, an alkenylene group which may have a substituent, an arylene group which may have a substituent, -O-, -NRx-, -CO-, -CS-, -SO-, -SO2-, or a divalent group formed by combining a plurality of these, and more preferably a single bond, an alkylene group which may have a substituent, an arylene group which may have a substituent, or a divalent group formed by combining a plurality of these.

[0127] The substituent that the divalent group in L may have is as described above, but from the viewpoint of further enjoying the effects of the present invention, it is preferably one or more selected from a halogen atom and a hydrocarbon group, more preferably one or more selected from a halogen atom, an alkyl group, and an aryl group, and even more preferably one or more selected from a fluorine atom, an alkyl group having 1 to 6 carbon atoms, and an aryl group having 6 to 10 carbon atoms.

[0128] The divalent linking group represented by L preferably has 60 or less carbon atoms, more preferably 48 or less, even more preferably 36 or less, and even more preferably 24 or less carbon atoms.

[0129] In particular, from the viewpoint of providing a cured product exhibiting good dielectric properties, the divalent linking group represented by L is preferably an alkylene group having 1 to 6 carbon atoms or a divalent group represented by the following formula (A4-4):

[0130] [ka] In formula (A4-4), R 1 ~R 8 each independently represents a hydrogen atom, an alkyl group having 1 to 6 carbon atoms, or a phenyl group; * represents a bond.

[0131] In formula (A4-4), R 1 ~R 8 each independently represents a hydrogen atom, an alkyl group having 1 to 6 carbon atoms, or a phenyl group. Among these, from the viewpoint of obtaining the effects of the present invention, R 1 , R 2 , R 7 and R 8 Preferably, R represents an alkyl group having 1 to 6 carbon atoms, and more preferably an alkyl group having 1 to 4 carbon atoms. 3 and R 4 Among these, it is preferable that one of them represents a hydrogen atom and the other represents an alkyl group having 1 to 6 carbon atoms, and R 5 and R 6 Of these, it is preferable that one represents a hydrogen atom and the other represents an alkyl group having 1 to 6 carbon atoms.

[0132] In formula (A4-2), R and m are as described above for the phenylene ether unit of formula (A4-1). Among them, the phenylene ether unit constituting the polyphenylene ether skeleton represented by formula (A4-2) is preferably a 2,6-disubstituted-1,4-phenylene ether unit, more preferably a 2,6-dialkyl-1,4-phenylene ether unit, a 2-alkyl-6-aryl-1,4-phenylene ether unit, a 2,6-diaryl-1,4-phenylene ether unit, or a 2,6-dihalo-1,4-phenylene ether unit, from the viewpoint of being able to enjoy the effects of the present invention.

[0133] In formula (A4-2), n1 and n2 each independently represent an integer in the range of 1 to 100.

[0134] In formula (A4-2), X's each independently represent (i) a (meth)acryloyl group, or (ii) a divalent group represented by formula (A4-3) above, where the term "(meth)acryloyl group" encompasses both a methacryloyl group and an acryloyl group, and the term "(meth)acryloyloxy group" encompasses both a methacryloyloxy group and an acryloyloxy group.

[0135] The case where X represents a divalent group represented by the above formula (A4-3), that is, the above embodiment (ii), will be described below.

[0136] In formula (A4-3), R, including preferred examples thereof, is as described above for the phenylene ether unit in formula (A4-1).

[0137] In formula (A4-3), A represents an alkylene group which may have a substituent. The alkylene group in A may be either linear or branched, and the number of carbon atoms is preferably 1 to 10, more preferably 1 to 6, and even more preferably 1 to 3. The substituent which the alkylene group may have is as described above, and among them, from the viewpoint of further enjoying the effects of the present invention, one or more types selected from a halogen atom and a hydrocarbon group are preferable, one or more types selected from a halogen atom, an alkyl group, and an aryl group are more preferable, and one or more types selected from a fluorine atom, an alkyl group having 1 to 6 carbon atoms, and an aryl group having 6 to 10 carbon atoms are even more preferable.

[0138] In formula (A4-3), Y represents an alkenyl group or a (meth)acryloyloxy group. The alkenyl group represented by Y may be either linear or branched, and has preferably 2 to 10 carbon atoms, more preferably 2 to 6, and further preferably 2 or 3. From the viewpoint of being able to enjoy the effects of the present invention more effectively in combination with resin X, the alkenyl group represented by Y is preferably a vinyl group or an allyl group.

[0139] In formula (A4-3), m1 represents an integer of 0 to 4, preferably 0 to 2, more preferably 0 or 1, and even more preferably 0.

[0140] As the terminal double bond modified polyphenylene ether resin, a commercially available product may be used, for example, "NORYL SA9000" manufactured by Sabic and "OPE-2St" manufactured by Mitsubishi Gas Chemical Company, Inc.

[0141] -Allyl resin- The allyl resin is a compound having at least one allyl group in the molecule. The allyl resin is not particularly limited in type as long as it has one or more allyl groups in one molecule, and may be a monomer or an oligomer. The allyl resin preferably has one or more allyl groups per molecule, more preferably has two or more allyl groups. The lower limit is not particularly limited, but it may be preferably 10 or less, more preferably 5 or less.

[0142] From the viewpoint of significantly obtaining the desired effects of the present invention, the allyl resin contained in the resin composition of the present invention preferably contains, in addition to the allyl group, a ring structure in the main skeleton, and the ring structure is selected from any one of a benzoxazine ring, a phenol ring, an isocyanuric ring, an epoxy group, and a carboxylic acid derivative having a ring structure.

[0143] The allyl resin having a benzoxazine ring is preferably bonded to either the nitrogen atom of the benzoxazine ring or the benzene ring, and more preferably bonded to the nitrogen atom.

[0144] Examples of allyl resins having a phenol ring include cresol resins containing an allyl group, novolac-type phenol resins containing an allyl group, and cresol novolac resins containing an allyl group.

[0145] In the allyl resin having an isocyanuric structure, a nitrogen atom of the isocyanuric structure and an allyl group are preferably directly bonded to each other. Examples of the allyl resin having an isocyanuric structure include allyl isocyanurate, diallyl isocyanurate, and triallyl isocyanurate.

[0146] The allyl resin having epoxy group preferably contains two or more epoxy groups in one molecule.The allyl resin having epoxy group preferably has an aromatic ring structure, and when using two or more allyl resins having epoxy group, at least one of them is more preferably aromatic ring structure.The allyl resin having epoxy group preferably has a bisphenol structure, and the bisphenol structure may be, for example, bisphenol A type, bisphenol F type, bisphenol AF type, etc.

[0147] The allyl resin having a carboxylic acid derivative having a ring structure is preferably an allyl carboxylate having a ring structure. The ring structure may be either a cyclic group containing an alicyclic structure or a cyclic group containing an aromatic ring structure. In addition, the cyclic group may have a ring skeleton formed by heteroatoms other than carbon atoms. Examples of the heteroatom include an oxygen atom, a sulfur atom, and a nitrogen atom, and nitrogen atoms are preferred. The ring may have one or more heteroatoms.

[0148] Examples of carboxylic acids having a ring structure include isocyanuric acid, diphenic acid, phthalic acid, cyclohexanedicarboxylic acid, etc. Examples of allyl resins having a carboxylic acid derivative having a ring structure include allyl isocyanurate, diallyl isocyanurate, triallyl isocyanurate, diallyl diphenate, allyl diphenate, ortho-diallyl phthalate, meth-diallyl phthalate, para-diallyl phthalate, allyl cyclohexanedicarboxylate, diallyl cyclohexanedicarboxylate, etc.

[0149] The allyl resin may be a commercially available product. Examples of commercially available products include "MEH-8000H" and "MEH-8005" (allyl resin having a phenol ring) manufactured by Meiwa Kasei Co., Ltd.; "RE-810NM" (allyl resin having an epoxy group) manufactured by Nippon Kayaku Co., Ltd.; "ALP-d" (allyl resin having a benzoxazine ring) manufactured by Shikoku Kasei Kogyo Co., Ltd.; "L-DAIC" (allyl resin having an isocyanuric ring) manufactured by Shikoku Kasei Kogyo Co., Ltd.; "TAIC" (allyl resin having an isocyanuric ring (triallyl isocyanurate) manufactured by Nippon Kasei Co., Ltd.; "MDAC" (allyl resin having a cyclohexanedicarboxylic acid derivative) manufactured by Osaka Soda Co., Ltd.; "DAD" (diallyl diphenate) manufactured by Nissho Techno Fine Chemical Co., Ltd.; and "Daiso DAP Monomer" (ortho-diallyl phthalate) manufactured by Osaka Soda Co., Ltd.

[0150] From the viewpoint of significantly obtaining the desired effects of the present invention, the allyl group equivalent of the allyl resin is preferably 20 g / eq. to 1000 g / eq., more preferably 50 g / eq. to 500 g / eq., and further preferably 100 g / eq. to 300 g / eq. The allyl group equivalent is the mass of the allyl resin containing one equivalent of an allyl group.

[0151] -Propenyl resin- The propenyl resin is a compound having at least one propenyl group (1-propenyl group) in the molecule. The propenyl resin may be a monomer or an oligomer as long as it has one or more propenyl groups in one molecule. The propenyl resin preferably has one or more propenyl groups per molecule, and more preferably has two or more propenyl groups.

[0152] The propenyl resin contained in the resin composition of the present invention contains a ring structure in the main skeleton in addition to the propenyl group, from the viewpoint of significantly obtaining the desired effects of the present invention, and a suitable ring structure is an indene ring. The propenyl resin may contain, in addition to an indene ring in the main skeleton, an aromatic ring such as styrene, vinyltoluene, etc. The propenyl resin that can be contained in the resin composition of the present invention is an aliphatic / aromatic copolymerized hydrocarbon resin. Examples of commercially available propenyl resins include Petrotac 70 and Petrotac 90 manufactured by Tosoh Corporation.

[0153] -(Meth)acrylic resin- The (meth)acrylic resin is a compound containing an acryloyl group, a methacryloyl group, and a combination thereof. In order to significantly obtain the desired effects of the present invention, the (meth)acrylic resin preferably has two or more (meth)acryloyl groups per molecule. The term "(meth)acryloyl group" includes an acryloyl group, a methacryloyl group, and a combination thereof.

[0154] The (meth)acrylic resin contained in the resin composition of the present invention has a ring structure in the main skeleton. The ring structure is preferably a divalent cyclic group. The divalent cyclic group may be either a cyclic group containing an alicyclic structure or a cyclic group containing an aromatic ring structure. Among them, from the viewpoint of significantly obtaining the desired effects of the present invention, a cyclic group containing an alicyclic structure is preferable.

[0155] From the viewpoint of significantly obtaining the desired effects of the present invention, the divalent cyclic group is preferably a 3-membered or larger ring, more preferably a 4-membered or larger ring, and even more preferably a 5-membered or larger ring, and is preferably a 20-membered or smaller ring, more preferably a 15-membered or smaller ring, and even more preferably a 10-membered or smaller ring. In addition, the divalent cyclic group may be a monocyclic structure or a polycyclic structure.

[0156] The ring in the divalent cyclic group may have a ring skeleton constituted by a heteroatom other than carbon atoms. Examples of the heteroatom include an oxygen atom, a sulfur atom, and a nitrogen atom, and an oxygen atom is preferred. The ring may have one or more heteroatoms.

[0157] Specific examples of the divalent cyclic group include the following divalent groups (i) to (xi). Among them, the divalent cyclic group is preferably (x) or (xi).

[0158] [ka]

[0159] The divalent cyclic group may have a substituent, such as a halogen atom, an alkyl group, an alkoxy group, an aryl group, an arylalkyl group, a silyl group, an acyl group, an acyloxy group, a carboxy group, a sulfo group, a cyano group, a nitro group, a hydroxy group, a mercapto group, or an oxo group, and an alkyl group is preferred.

[0160] The (meth)acryloyl group may be directly bonded to the divalent cyclic group, or may be bonded via a divalent linking group. Examples of the divalent linking group include an alkylene group, an alkenylene group, an arylene group, a heteroarylene group, -C(=O)O-, -O-, -NHC(=O)-, -NC(=O)N-, -NHC(=O)O-, -C(=O)-, -S-, -SO-, -NH-, and the like, and may be a group in which a plurality of these are combined. The alkylene group is preferably an alkylene group having 1 to 10 carbon atoms, more preferably an alkylene group having 1 to 6 carbon atoms, and even more preferably an alkylene group having 1 to 5 carbon atoms or an alkylene group having 1 to 4 carbon atoms. The alkylene group may be linear, branched, or cyclic. Examples of such alkylene groups include methylene, ethylene, propylene, butylene, pentylene, hexylene, and 1,1-dimethylethylene groups, and are preferably methylene, ethylene, or 1,1-dimethylethylene. As the alkenylene group, an alkenylene group having 2 to 10 carbon atoms is preferred, an alkenylene group having 2 to 6 carbon atoms is more preferred, and an alkenylene group having 2 to 5 carbon atoms is even more preferred. As the arylene group or heteroarylene group, an arylene group or heteroarylene group having 6 to 20 carbon atoms is preferred, and an arylene group or heteroarylene group having 6 to 10 carbon atoms is more preferred. As the divalent linking group, an alkylene group is preferred, and among them, a methylene group or a 1,1-dimethylethylene group is preferred.

[0161] The (meth)acrylic resin is preferably represented by the following formula (A5-1).

[0162] [ka] (In formula (A5-1), R 101 and R 104 each independently represents an acryloyl group or a methacryloyl group, R 102 and R 103 each independently represents a divalent linking group. Ring B2 represents a divalent cyclic group.

[0163] R101 and R 104 each independently represents an acryloyl group or a methacryloyl group, and an acryloyl group is preferred.

[0164] R 102 and R 103 each independently represents a divalent linking group. The divalent linking group is the same as the divalent linking group which may have a (meth)acryloyl group bonded thereto.

[0165] Ring B2 represents a divalent cyclic group. Ring B2 is the same as the divalent cyclic group. Ring B2 may have a substituent. The substituent is the same as the substituent that the divalent cyclic group may have.

[0166] Specific examples of the (meth)acrylic resin include the following, but the present invention is not limited thereto.

[0167] [ka]

[0168] As the (meth)acrylic resin, commercially available products may be used, and examples thereof include "A-DOG" manufactured by Shin-Nakamura Chemical Co., Ltd., "DCP-A" manufactured by Kyoeisha Chemical Co., Ltd., "NPDGA", "FM-400", "R-687", "THA230", "PET-30", and "DPHA" manufactured by Nippon Kayaku Co., Ltd., and "NK Ester DCP" manufactured by Shin-Nakamura Chemical Co., Ltd.

[0169] As described above, the radical polymerizable resin A contained in the resin composition of the present invention can be a compound containing a ring structure in the main skeleton and containing a radical polymerizable unsaturated group that exhibits radical polymerization activity by the action of a free radical, and such a compound is preferably any one of maleimide resin, terminal double bond modified polyphenylene ether resin, allyl resin, and (meth)acrylic resin. In addition, from the viewpoint of being able to enjoy the effects of the present invention more in combination with di-t-amyl peroxide, the radical polymerizable resin A preferably contains two or more radical polymerizable resins, and in that case, it is more preferable to contain at least a resin selected from the group consisting of maleimide resin, terminal double bond modified polyphenylene ether resin, and (meth)acrylic resin. As the terminal double bond modified polyphenylene ether resin, a polyphenylene ether resin in which the molecular end is modified by a phenyl group substituted with a vinyl group or an allyl group is preferable.

[0170] From the viewpoint of obtaining the effects of the present invention and realizing film properties with good handleability when uncured, it is preferable that the radical polymerizable resin A contains a radical polymerizable resin having a molecular weight (weight average molecular weight when it has a distribution) of 1,000 or less. More preferably, it contains a radical polymerizable resin having a molecular weight of 800 or less, even more preferably a molecular weight of 600 or less, and even more preferably a molecular weight of 500 or less, or 400 or less. The lower limit of the molecular weight is not particularly limited, and may be, for example, 150 or more, 200 or more, etc. The weight average molecular weight (when it has a distribution) of the radical polymerizable resin is based on a polystyrene-equivalent value measured by gel permeation chromatography (GPC).

[0171] As the radical polymerizable resin having a molecular weight of 1,000 or less, any of the above-mentioned radical polymerizable resins having a molecular weight of 1,000 or less may be used, such as "DAD" manufactured by Nisshoku Techno Fine Chemical Co., Ltd., "A-DOG" manufactured by Shin-Nakamura Chemical Co., Ltd., and "DCP-A" manufactured by Kyoeisha Chemical Co., Ltd.

[0172] From the viewpoint of being able to enjoy the effects of the present invention more in combination with di-t-amyl peroxide, it is preferable that the radical polymerizable resin A contains a radical polymerizable resin (A-1) having an active group equivalent of 250 g / eq. or more in combination with a radical polymerizable resin (A-2) having an active group equivalent of less than 250 g / eq. The active group equivalent of the radical polymerizable resin (A-1) is preferably 250 g / eq. or more, more preferably 300 g / eq. or more, even more preferably 350 g / eq. or more, 400 g / eq. or more, 450 g / eq. or more, or 500 g / eq. or more. The upper limit of the active group equivalent of the radical polymerizable resin (A-1) is not particularly limited, and may be, for example, 2000 g / eq. or less, 1800 g / eq. or less, 1600 g / eq. or less, or 1500 g / eq. or less. In order to easily achieve better film properties when uncured in combination with the radical polymerizable resin (A-1), the active group equivalent of the radical polymerizable resin (A-2) is preferably less than 250 g / eq., more preferably 240 g / eq. or less, even more preferably 220 g / eq. or less, 200 g / eq. or less, or 180 g / eq. or less.

[0173] From the viewpoint of enhancing the intended effect of the present invention, the content of the radical polymerizable resin A is preferably 20% by mass or more, more preferably 30% by mass or more, even more preferably 40% by mass or more, 50% by mass or more, 60% by mass or more, still more preferably 70% by mass or more, 80% by mass or more, 85% by mass or more, or 90% by mass or more, based on 100% by mass of the resin component in the resin composition. The upper limit of the content is not particularly limited, and may be, for example, 99% by mass or less, 98% by mass or less, etc.

[0174] In the present invention, the term "resin component" in relation to the resin composition refers to the non-volatile components constituting the resin composition excluding the inorganic filler.

[0175] The content of the radical polymerizable resin (A-1) and the radical polymerizable resin (A-2) in the radical polymerizable resin A is preferably such that the content of the radical polymerizable resin (A-1) is greater than the content of the radical polymerizable resin (A-2) (i.e., the content of the radical polymerizable resin (A-2) is less) from the viewpoint of significantly enjoying the effects of the present invention in combination with di-t-amyl peroxide. The content ratio of the radical polymerizable resin (A-1) to the radical polymerizable resin (A-2) is preferably such that the content of the radical polymerizable resin (A-1) is 50% or less, more preferably 30% or less, and even more preferably 20% or less, 18% or less, 16% or less, or 15% or less.

[0176] <Di-t-amyl peroxide> The resin composition of the present invention contains di-t-amyl peroxide, which is a compound represented by the following formula and generates free radicals when heated.

[0177] [ka]

[0178] Di-t-amyl peroxide acts as a polymerization initiator, acting on the radically polymerizable unsaturated groups contained in the radically polymerizable resin A to initiate polymerization. As the di-t-amyl peroxide, commercially available products can be used, for example, "Luperox DTA" manufactured by Arkema Yoshitomi Co., Ltd.

[0179] From the viewpoint of providing a cured product having excellent resin flatness and good dielectric properties and peel strength, when the resin component in the resin composition is taken as 100% by mass, the content of di-t-amyl peroxide in the resin composition is preferably 0.1% by mass or more, more preferably 0.3% by mass or more, even more preferably 0.5% by mass or more, 0.7% by mass or more, 0.9% by mass or more, or 1% by mass or more. From the same viewpoint, the upper limit of the content is preferably 5% by mass or less, more preferably 4% by mass or less or 3% by mass or less, even more preferably 2.5% by mass or less, 2.0% by mass or less, 1.8% by mass or less, 1.6% by mass or less, or 1.5% by mass or less. Therefore, in one embodiment, when the resin component in the resin composition is taken as 100% by mass, the content of di-t-amyl peroxide in the resin composition is 0.1% by mass or more and 2.5% by mass or less.

[0180] <Inorganic filler> The resin composition of the present invention preferably contains an inorganic filler, which can achieve better dielectric properties.

[0181] Examples of inorganic fillers include silica, alumina, glass, cordierite, silicon oxide, barium sulfate, barium carbonate, talc, clay, mica powder, zinc oxide, hydrotalcite, boehmite, aluminum silicate, 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. Among these, silica is particularly suitable. Examples of silica include amorphous silica, fused silica, crystalline silica, synthetic silica, and hollow silica. In addition, spherical silica is preferred as the silica. The inorganic filler may be used alone or in combination of two or more.

[0182] The average particle size of the inorganic filler is not particularly limited, but is preferably 10 μm or less, more preferably 5 μm or less, even more preferably 3 μm or less, 2 μm or less, 1 μm or less, or 0.7 μm or less. The lower limit of the average particle size is not particularly limited, but is preferably 0.01 μm or more, more preferably 0.05 μm or more, even more preferably 0.07 μm or more, 0.1 μm or more, or 0.2 μm or more. The average particle size of the inorganic filler can be measured by a laser diffraction / scattering method based on the Mie scattering theory. Specifically, the particle size distribution of the inorganic filler is created on a volume basis using a laser diffraction / scattering particle size distribution measuring device, and the median diameter is used as the average particle size. The measurement sample can be prepared by weighing 100 mg of the inorganic filler and 10 g of methyl ethyl ketone into a vial and dispersing it by ultrasonic waves for 10 minutes. The measurement sample is measured using a laser diffraction particle size distribution measuring device with blue and red light source wavelengths used, and the volume-based particle size distribution of the inorganic filler is measured using a flow cell method, and the average particle size is calculated as the median diameter from the particle size distribution obtained. An example of a laser diffraction particle size distribution measuring device is the "LA-960" manufactured by Horiba, Ltd.

[0183] The specific surface area of ​​the inorganic filler is not particularly limited, but is preferably 0.1 m 2 / g or more, more preferably 0.5m 2 / g or more, more preferably 1m 2 / g or more, 3m 2 / g or more or 5m 2 The upper limit of the specific surface area is not particularly limited, but is preferably 100 m 2 / g or less, more preferably 80m 2 / g or less, more preferably 60m 2 / g or less, 50m 2 / g or less or 40m 2 / g or less. The specific surface area of ​​the inorganic filler is obtained according to the BET method by adsorbing nitrogen gas onto the surface of the sample using a specific surface area measuring device (Macsorb HM-1210 manufactured by Mountec Co., Ltd.) and calculating the specific surface area using the BET multipoint method.

[0184] The inorganic filler may be a non-hollow inorganic filler with a porosity of 0 volume % (preferably non-hollow silica), or a hollow inorganic filler with a porosity of more than 0 volume % (preferably hollow silica), or may include both. The porosity of the hollow inorganic filler is preferably 70 volume % or less, more preferably 60 volume % or less or 50 volume % or less. The lower limit of the porosity of the inorganic filler may be, for example, more than 0 volume %, 1 volume % or more, 5 volume % or more, 10 volume % or more, etc. The porosity P (volume %) of the inorganic filler is defined as the volume-based ratio of the total volume of one or more voids present inside the particle to the total volume of the particle based on the outer surface of the particle (total volume of voids / volume of particle), and is, for example, a measured value D of the actual density of the inorganic filler. M (g / cm 3 ), and the theoretical value of the material density of the material forming the inorganic filler D T (g / cm 3 ) is used to calculate the following formula (1):

[0185]

number

[0186] The actual density of the inorganic filler can be measured, for example, by using a true density measuring device. Examples of the true density measuring device include ULTRAPYCNOMETER 1000 manufactured by QUANTACHROME Co., Ltd. As the measurement gas, for example, nitrogen is used.

[0187] Examples of commercially available inorganic fillers include "SP60-05" and "SP507-05" manufactured by Nippon Steel Chemical & Material Co., Ltd.; "YC100C", "YA050C", "YA050C-MJE", "YA010C", "SC2500SQ", "SO-C4", "SO-C2", and "SO-C1" manufactured by Admatechs Co., Ltd.; "UFP-30", "DAW-03", and "FB-105FD" manufactured by Denka Co., Ltd.; "Silfil NSS-3N", "Silfil NSS-4N", and "Silfil NSS-5N" manufactured by Tokuyama Corporation; "Cellspheres" and "MGH-005" manufactured by Pacific Cement Corporation; "Sferique" and "BA-1" manufactured by JGC Catalysts and Chemicals Co., Ltd.; and "Hipressica FH" manufactured by Ube Exsymo Co., Ltd.

[0188] The inorganic filler is preferably surface-treated with a suitable surface treatment agent. By performing the surface treatment, the moisture resistance and dispersibility of the inorganic filler can be improved. Examples of the surface treatment agent include silane coupling agents such as vinyl silane coupling agents, epoxy silane coupling agents, styryl silane coupling agents, (meth)acrylic silane coupling agents, amino silane coupling agents, isocyanurate silane coupling agents, ureido silane coupling agents, mercapto silane coupling agents, isocyanate silane coupling agents, and acid anhydride silane coupling agents; non-silane coupling-alkoxysilane compounds such as methyltrimethoxysilane and phenyltrimethoxysilane; and silazane compounds. The surface treatment agent may be used alone or in combination of two or more.

[0189] Examples of commercially available surface treatment agents include Shin-Etsu Chemical Co., Ltd.'s "KBM403" (3-glycidoxypropyltrimethoxysilane), Shin-Etsu Chemical Co., Ltd.'s "KBM803" (3-mercaptopropyltrimethoxysilane), Shin-Etsu Chemical Co., Ltd.'s "KBE903" (3-aminopropyltriethoxysilane), Shin-Etsu Chemical Co., Ltd.'s "KBM573" (N-phenyl-3-aminopropyltrimethoxysilane), and Shin-Etsu Chemical Co., Ltd.'s "SZ-31" (hexamethyldisilazane).

[0190] The degree of surface treatment with the surface treatment agent is preferably within a predetermined range from the viewpoint of improving the dispersibility of the inorganic filler. Specifically, it is preferable that 100% by mass of the inorganic filler is surface-treated with 0.2 to 5% by mass of the surface treatment agent.

[0191] The degree of surface treatment with the surface treatment agent can be evaluated by the amount of carbon per unit surface area of ​​the inorganic filler. From the viewpoint of improving the dispersibility of the inorganic filler, the amount of carbon per unit surface area of ​​the inorganic filler is set to 0.02 mg / m 2 More than 0.1 mg / m is preferable. 2 More preferably, 0.2 mg / m or more 2 On the other hand, from the viewpoint of preventing an increase in the melt viscosity of the resin composition or the melt viscosity in the form of a sheet, it is more preferable that the melt viscosity is 1.0 mg / m 2 Less than 0.8 mg / m is preferred. 2 Less than 0.5 mg / m is more preferable. 2 The following is more preferable. 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 (e.g., methyl ethyl ketone (MEK)). Specifically, a sufficient amount of MEK as a solvent is added to the inorganic filler that has been surface-treated with a surface treatment agent, and ultrasonic cleaning is performed at 25°C for 5 minutes. After removing the supernatant and drying the solid content, the amount of carbon per unit surface area of ​​the inorganic filler can be measured using a carbon analyzer. As the carbon analyzer, an "EMIA-320V" manufactured by Horiba, Ltd., or the like can be used.

[0192] In the combination of the radical polymerizable resin A and di-t-amyl peroxide, from the viewpoint of being able to enjoy the effects of the present invention more, particularly from the viewpoint of providing a cured product with excellent dielectric properties, the content of the inorganic filler in the resin composition is preferably 30% by mass or more, 40% by mass or more, 50% by mass or more, more preferably 55% by mass or more, and even more preferably 60% by mass or more, 62% by mass or more, 64% by mass or more, or 65% by mass or more, when the non-volatile components in the resin composition are taken as 100% by mass. The upper limit of the content of the inorganic filler is not particularly limited, but may be, for example, 90% by mass or less, 85% by mass or less, etc.

[0193] <Thermoplastic resin> The resin composition of the present invention may further contain a thermoplastic resin, except for those that fall under the radical polymerizable resin A.

[0194] Examples of the thermoplastic resin include phenoxy resin, polyimide resin, polyvinyl acetal resin, acrylic resin, polyolefin resin, polybutadiene resin, polyamideimide resin, polysulfone resin, polyethersulfone resin, polyphenylene ether resin, polyetherimide resin, polycarbonate resin, polyetheretherketone resin, and polyester resin, and among them, a resin selected from phenoxy resin, polyimide resin, acrylic resin, polyphenylene ether resin, and polycarbonate resin is preferable. The thermoplastic resin may be used alone or in combination of two or more kinds.

[0195] [Phenoxy resin] Examples of the phenoxy resin include phenoxy resins having one or more skeletons selected from the group consisting of bisphenol A skeleton, bisphenol F skeleton, bisphenol S skeleton, bisphenolacetophenone skeleton, novolac skeleton, biphenyl skeleton, fluorene skeleton, dicyclopentadiene skeleton, norbornene skeleton, naphthalene skeleton, anthracene skeleton, adamantane skeleton, terpene skeleton, and trimethylcyclohexane skeleton. The terminal of the phenoxy resin may be any functional group such as a phenolic hydroxyl group or an epoxy group. The phenoxy resin may be used alone or in combination of two or more. Specific examples of phenoxy resins include "1256" and "4250" (both of which are phenoxy resins containing a bisphenol A skeleton), "YX8100" (phenoxy resin containing a bisphenol S skeleton), and "YX6954" (phenoxy resin containing a bisphenol acetophenone skeleton) manufactured by Mitsubishi Chemical Corporation, "FX280" and "FX293" manufactured by Nippon Steel Chemical & Material Co., Ltd., and "YX7200B35", "YX7500BH30", "YX6954BH30", "YX7553", "YX7553BH30", "YL7769BH30", "YL6794", "YL7213", "YL7290", and "YL7482" manufactured by Mitsubishi Chemical Corporation.

[0196] -Polyimide resin- The polyimide resin may be a resin having an imide structure. The polyimide resin may generally be obtained by the imidization reaction between a diamine compound and an acid anhydride, or the imidization reaction between a diisocyanate compound and an acid anhydride. Specific examples of the polyimide resin include modified polyimides such as linear polyimides (polyimides described in JP-A-2006-37083) obtained by reacting a difunctional hydroxyl group-terminated polybutadiene, a diisocyanate compound, and a tetrabasic acid anhydride, and polysiloxane skeleton-containing polyimides (polyimides described in JP-A-2002-12667 and JP-A-2000-319386). The polyimide resin may be a commercially available product, such as "Rikacoat SN20" and "Rikacoat PN20" manufactured by New Japan Chemical Co., Ltd.

[0197] Particularly preferred examples of polyimide resins are shown below. In a preferred embodiment, the polyimide resin contains a structural unit represented by the following formula (C1) (hereinafter also referred to as "structural unit (1)"). The number of structural units (1) contained per molecule of the polyimide resin is 1 or more, and is not particularly limited, but may be 100 or less, 50 or less, or 30 or less.

[0198] [ka] [In formula (C1), R1 is a tetravalent group represented by the following formula (C1-1): R2 is a divalent group represented by the following formula (C1-2).

[0199] [ka] (In formula (C1-1), Ar 11 , Ar 12 , Ar 13 and Ar 14 each independently represents an aromatic ring which may have a substituent, L 11 , L 12 and L 13 each independently represents a divalent linking group, nc1 represents an integer equal to or greater than 0.)

[0200] [ka] (In formula (C1-2), Ar 21 , Ar 22 , Ar 23 and Ar 24 each independently represents an aromatic ring which may have a substituent, L 21 , L 22 and L 23 each independently represents a divalent linking group, nc2 represents an integer equal to or greater than 1. )]

[0201] In formula (C1-1), Ar 11 , Ar 12 , Ar 13 and Ar 14 The aromatic ring represented by (hereinafter also referred to as "aromatic ring C") is preferably an aromatic ring having 6 to 100 carbon atoms, more preferably 6 to 50 carbon atoms, still more preferably 6 to 100 carbon atoms, still more preferably 6 to 50 carbon atoms. 11 , Ar 12 , Ar 13 and Ar 14 are each independently an aromatic carbocyclic ring having 6 to 14 carbon atoms which may have a substituent. In this specification, the term "aromatic ring" means a ring according to the Huckel rule in which the number of electrons contained in the π electron system on the ring is 4n+2 (n is a natural number), and includes a monocyclic aromatic ring and a fused aromatic ring in which two or more monocyclic aromatic rings are fused. The aromatic ring may be a carbocyclic ring or a heterocyclic ring. Examples of the aromatic ring include monocyclic aromatic rings such as a benzene ring, a furan ring, a thiophene ring, a pyrrole ring, a pyrazole ring, an oxazole ring, an isoxazole ring, a thiazole ring, an imidazole ring, a pyridine ring, a pyridazine ring, a pyrimidine ring, and a pyrazine ring; fused rings in which two or more monocyclic aromatic rings are fused, such as a naphthalene ring, an anthracene ring, a benzofuran ring, an isobenzofuran ring, an indole ring, an isoindole ring, a benzothiophene ring, a benzimidazole ring, an indazole ring, a benzoxazole ring, a benzisoxazole ring, a benzothiazole ring, a quinoline ring, an isoquinoline ring, a quinoxaline ring, an acridine ring, a quinazoline ring, a cinnoline ring, and a phthalazine ring; and fused rings in which one or more monocyclic aromatic rings are fused to one or more monocyclic non-aromatic rings, such as an indane ring, a fluorene ring, and a tetralin ring. Among these, an aromatic carbon ring having 6 to 14 carbon atoms is preferred, and a benzene ring is more preferred.

[0202] In formula (C1-1), Ar 11 , Ar 12 , Ar 13 and Ar 14When represents an aromatic ring having a substituent, the number of the substituent is not limited. Such a substituent (hereinafter also referred to as "substituent S") may be, independently of one another, a halogen atom, an alkyl group, a cycloalkyl group, an alkoxy group, a cycloalkyloxy group, an aryl group, an aryloxy group, an arylalkyl group, an arylalkoxy group, a monovalent heterocyclic group, an alkylidene group, an amino group, a silyl group, an acyl group, an acyloxy group, a carboxy group, a sulfo group, a cyano group, a nitro group, a hydroxy group, a mercapto group, and an oxo group.

[0203] In formula (C1-1), L 11 , L 12 and L 13 The divalent linking group represented by is preferably a divalent group consisting of one or more (for example, 1 to 3000, 1 to 1000, 1 to 100, 1 to 50) skeletal atoms selected from carbon atoms, oxygen atoms, nitrogen atoms, sulfur atoms, and silicon atoms. Examples of the divalent linking group include -SO2-, -CO-, -COO-, -O-, -S-, -O-C6H4-O- (wherein -C6H4- represents a phenylene group), -O-C6H4-C(CH3)2-C6H4-O-, -COO-(CH2) q -OCO- (wherein q represents an integer of 1 to 20), -COO-H2C-HC(-OC(=O)-CH3)-CH2-OCO-, an alkylene group, an alkenylene group, an alkynylene group, an arylene group, a heteroarylene group, -C(=O)-, -C(=O)-O-, -NR 0 - (where R 0 represents a hydrogen atom or an alkyl group having 1 to 3 carbon atoms; and -C(=O)-NR 0The number of carbon atoms in the alkylene group is preferably 1 to 10, more preferably 1 to 6, and even more preferably 1 to 5 or 1 to 4. The number of carbon atoms in the alkenylene group is preferably 2 to 10, more preferably 2 to 6, and even more preferably 2 to 5. The number of carbon atoms in the arylene group is preferably 6 to 20, more preferably 6 to 10, and the number of carbon atoms in the heteroarylene group is preferably 2 to 20, more preferably 3 to 10, 4 to 10, or 5 to 10. The above-mentioned alkyl group, alkylene group, alkenylene group, alkynylene group, arylene group, and heteroarylene group may further have a substituent. Examples of the substituent include the above-mentioned substituent S. L 11 , L 12 and L 13 In one embodiment, the divalent linking group represented by L preferably does not contain an aromatic ring. 11 A divalent linking group represented by 13 and the divalent linking group represented by 11 A divalent linking group represented by 12 In a preferred embodiment, in formula (C1-1), L 11 and L 13 is -O- and L 12 is an alkylene group which may have a substituent, and in a more preferred embodiment, in formula (C1-1), Ar 11 , Ar 12 , Ar 13 and Ar 14 are each independently an aromatic carbocyclic ring having 6 to 14 carbon atoms which may have a substituent, and L 11 and L 13 is -O- and L 12 In a further preferred embodiment, in formula (C1-1), L 11 and L 13 is -O- and L 12 is a dimethylmethylene group.

[0204] In formula (C1-2), Ar 21 , Ar 22 , Ar 23 and Ar 24Examples of the aromatic ring represented by and the substituent that the aromatic ring may have are the same as those of the aromatic ring C and the substituent S, respectively. Therefore, in a preferred embodiment, in formula (C1-2), Ar 21 , Ar 22 , Ar 23 and Ar 24 are each independently an aromatic carbon ring having 6 to 14 carbon atoms which may have a substituent. 21 and L 23 is -O- and L 22 is an alkylene group which may have a substituent, and in a more preferred embodiment, in formula (C1-2), Ar 21 , Ar 22 , Ar 23 and Ar 24 are each independently an aromatic carbocyclic ring having 6 to 14 carbon atoms which may have a substituent, and L 21 and L 23 is -O- and L 22 In a further preferred embodiment, in formula (C1-2), L 21 and L 23 is -O- and L 22 is a dimethylmethylene group.

[0205] In a particularly preferred embodiment, in formula (C1-1), Ar 11 , Ar 12 , Ar 13 and Ar 14 are each independently an aromatic carbon ring having 6 to 14 carbon atoms which may have a substituent, and in formula (C1-2), Ar 21 , Ar 22 , Ar 23 and Ar 24 are each independently an aromatic carbon ring having 6 to 14 carbon atoms which may have a substituent. 11 and L 13 is -O- and L 12 is an alkylene group which may have a substituent, and in formula (C1-2), L 21and L 23 is -O- and L 22 is an alkylene group which may have a substituent.

[0206] In formula (C1-1), nc1 preferably represents an integer of 1 or more. The upper limit of the integer represented by nc1 is not particularly limited, but may be, for example, 50, 40, 30, or 20.

[0207] In formula (C1-2), nc2 preferably represents an integer of 2 or more. The upper limit of the integer represented by nc2 is not particularly limited, but may be, for example, 60, 50, 40, or 30.

[0208] The structural unit (C1) can be obtained, for example, by a known method for producing a polyimide resin, typically a method for imidizing a monomer composition containing a tetracarboxylic dianhydride and a diamine compound by polymerizing it, or a method for imidizing a monomer composition containing a tetracarboxylic dianhydride and a diisocyanate compound by polymerizing it. Note that it is permissible for the polyimide resin to partially contain a polyamic acid structure that may be generated during the imidization process.

[0209] The structural unit (C1) may be obtained, for example, by reacting 2,2-bis[4-(3,4-dicarboxyphenoxy)phenyl]propane dianhydride (a compound represented by the following formula (I); hereinafter, also referred to as "BPADA") with 4,4'-[1,4-phenylenebis[(1-methylethylidene)-4,1-phenyleneoxy]]bisbenzenamine (a compound represented by the following formula (II); hereinafter, also referred to as "BPPAN"). That is, R1 in the structural unit (1) is a skeleton derived from BPADA, and R2 is a skeleton derived from BPPAN.

[0210] [ka]

[0211] [ka]

[0212] The polyimide resin may further include a structural unit represented by the following formula (C2) (hereinafter also referred to as "structural unit (C2)"). Thus, in one embodiment, the polyimide resin further includes a structural unit represented by the following formula (C2). The number of structural units (C2) contained per molecule of the polyimide resin is 0 or more, and is not particularly limited, but may be 100 or less, 50 or less, or 30 or less.

[0213] [ka] (In formula (C2), R3 represents a tetravalent aliphatic group which may have a substituent or a tetravalent aromatic group which may have a substituent; R4 represents a divalent aliphatic group which may have a substituent or a divalent aromatic group which may have a substituent, provided that when R3 is the same as R1, R4 is different from R2, and when R4 is the same as R2, R3 is different from R1.

[0214] In formula (C2), the tetravalent aliphatic group represented by R3 contains at least a carbon atom, and is preferably a tetravalent group consisting of one or more (e.g., 1 to 3000, 1 to 1000, 1 to 100, 1 to 50) skeletal atoms selected from carbon atoms, oxygen atoms, nitrogen atoms, sulfur atoms, and silicon atoms. In formula (C2), the tetravalent aliphatic group represented by R3 is more preferably a tetravalent aliphatic group having 1 to 100 carbon atoms, and further preferably 1 to 50 carbon atoms. In formula (C2), when R3 represents a tetravalent aliphatic group having a substituent, examples of the substituent are the same as the examples of the substituent S.

[0215] In formula (C2), the tetravalent aromatic group represented by R3 is preferably a tetravalent aromatic group having 6 to 100 carbon atoms, more preferably 6 to 50 carbon atoms. The aromatic group contains at least an aromatic ring. Examples of the aromatic ring contained in the aromatic group include Ar 11 , Ar 12 , Ar 13 and Ar 14In formula (C2), when R3 represents a tetravalent aromatic group having a substituent, examples of the substituent are the same as the examples of the substituent S.

[0216] The tetravalent aromatic group represented by R3 may be a group obtained by removing two acid anhydride groups from a tetracarboxylic dianhydride having an aromatic group which may have a substituent. Specific examples of the tetracarboxylic dianhydride having an aromatic group which may have a substituent include BPADA, pyromellitic dianhydride, 3,3',4,4'-biphenyltetracarboxylic dianhydride, 4,4'-oxydiphthalic anhydride, 3,3',4,4'-benzophenonetetracarboxylic dianhydride, and 3,3',4,4'-diphenylsulfonetetracarboxylic dianhydride.

[0217] In formula (C2), the divalent aliphatic group represented by R4 contains at least a carbon atom, and is preferably a divalent group consisting of one or more (e.g., 1 to 3000, 1 to 1000, 1 to 100, 1 to 50) skeletal atoms selected from carbon atoms, oxygen atoms, nitrogen atoms, sulfur atoms, and silicon atoms. In formula (C2), the divalent aliphatic group represented by R4 is more preferably a divalent aliphatic group having 1 to 100 carbon atoms, and even more preferably a divalent aliphatic group having 1 to 50 carbon atoms. In formula (C2), when R4 represents a divalent aliphatic group having a substituent, examples of the substituent are the same as the examples of the substituent S, and are, for example, an alkyl group having 1 to 6 carbon atoms. Therefore, in one embodiment, R4 is a divalent aliphatic group which may have a substituent, and one of the substituents is an alkyl group having 1 to 6 carbon atoms. In one embodiment, R4 is a divalent aliphatic group which may have a substituent, and is a divalent group obtained by removing two amino groups from isophoronediamine.

[0218] When R4 represents a divalent aliphatic group which may have a substituent, it may be a group obtained by removing two amino groups from a diamine compound having a linear aliphatic group which may have a substituent selected from 1,2-diaminoethane, 1,3-diaminopropane, 1,4-diaminobutane, 1,5-diaminopentane, 1,6-hexanediamine, 1,7-heptanediamine, 1,8-octanediamine, 1,9-nonanediamine, 1,10-decanediamine, 1,11-undecanediamine, and 1,12-dodecanediamine.

[0219] When R4 represents a divalent aliphatic group which may have a substituent, it may be a group obtained by removing two amino groups from a diamine compound having a branched aliphatic group which may have a substituent selected from 1,2-diaminopropane, 1,2-diamino-2-methylpropane, 1,3-diamino-2-methylpropane, 1,3-diamino-2,2-dimethylpropane, 1,3-diaminopentane, and 1,5-diamino-2-methylpentane.

[0220] When R4 represents a divalent aliphatic group which may have a substituent, examples thereof include 5-amino-1,3,3-trimethylcyclohexanemethylamine (isophoronediamine), 1,4-diaminocyclohexane, 1,3-diaminocyclohexane, 1,4-cyclohexanebis(methylamine), 1,3-cyclohexanebis(methylamine), 4,4'-diaminodicyclohexylmethane, bis(4-amino-3-methylcyclohexyl)methane, 3(4),8(9)-bis(aminomethyl)tricyclo[5.2.1.0 2,6 ]decane, 2,5(6)-bis(aminomethyl)bicyclo[2.2.1]heptane, 1,3-diaminoadamantane, 3,3'-diamino-1,1'-biadamantyl, and 1,6-diaminoadamantane, from which two amino groups have been removed. These diamine compounds are characterized in that the aliphatic group contains an alicyclic carbon ring.

[0221] In formula (C2), the divalent aromatic group represented by R4 is preferably a divalent aromatic group having 6 to 100 carbon atoms, more preferably 6 to 50 carbon atoms. The aromatic group contains at least an aromatic ring. Examples of the aromatic ring contained in the aromatic group are the same as the examples of the aromatic ring C. In formula (C2), when R4 represents a divalent aromatic group having a substituent, examples of the substituent are the same as the examples of the substituent S.

[0222] When R4 represents a divalent aromatic group which may have a substituent, it may be a group obtained by removing two amino groups from a diamine compound having an aromatic group which may have a substituent selected from 4,4'-diaminodiphenyl ether, 1,4-phenylenediamine, and 2,2-bis[4-(4-aminophenoxy)phenyl]propane.

[0223] With the proviso that when R3 is the same as R1, R4 is different from R2, and when R4 is the same as R2, R3 is different from R1. In one embodiment, R3 is the same as R1.

[0224] The above-mentioned structural unit (2) can be obtained, for example, according to a known method for producing a polyimide resin. The structural unit (C2) can be obtained, for example, by reacting BPADA with isophoronediamine. That is, R3 in the structural unit (2) is a skeleton derived from BPADA, and R4 is a skeleton derived from isophoronediamine. When R3 is the same as R1, R3 and R1 are skeletons derived from BPADA.

[0225] The terminal structure of the polyimide resin is not particularly limited. For example, the terminal structure of the polyimide resin may be an acid anhydride group derived from the raw material compound (for example, an acid such as BPADA, an amine compound such as BPPAN), or a carboxyl group or an amino group. When the raw material compound further contains maleic anhydride, the terminal structure of the polyimide resin may be a maleimide group.

[0226] The glass transition temperature Tg (°C) of the polyimide resin is preferably 140°C or higher, more preferably 145°C or higher, and even more preferably 150°C or higher, 160°C or higher, or 170°C or higher. There is no particular upper limit, but it may be 300°C or lower. The glass transition temperature Tg (°C) of the polyimide resin can be measured by thermomechanical analysis (TMA).

[0227] The content of the structural unit (C1) in the polyimide resin is preferably 5% by mass or more, more preferably 10% by mass or more, and even more preferably 20% by mass or more, 30% by mass or more, or 40% by mass or more. The upper limit of the content can be, for example, 98% by mass or less, 95% by mass or less, 90% by mass or less, or 85% by mass or less. Here, the content (mass percentage) of the structural unit (C1) can be calculated from the ratio of the charged amount (parts by mass) of each material used in the synthesis of the polyimide resin. Alternatively, the molecular weight of the polyimide resin and the formula weight of the structural unit (C1) may be specified, and the content may be calculated as the ratio of the formula weight of the structural unit (C1) to the molecular weight. When the polyimide resin is a polymer, it is preferable that the content of the structural unit (C1) estimated from the degree of polymerization is within the above range.

[0228] When the polyimide resin further contains the structural unit (C2), the content of the structural unit (C2) may be 0% by mass (i.e., no structural unit (C2) is contained), and there is no upper limit as long as the effect of the present invention is not impaired. The content of the structural unit (C2) in the polyimide resin may be, for example, 1% by mass or more, 5% by mass or more, 10% by mass or more, 20% by mass or more, or 30% by mass or more, and 95% by mass or less, 90% by mass or less, 80% by mass or less, 70% by mass or less, or 60% by mass or less. Here, the content of the structural unit (C2) is calculated in the same manner as the content of the structural unit (C1).

[0229] The weight average molecular weight (Mw) of the polyimide resin is 1,000 or more, preferably 1,00 to 10,000, and more preferably 1,000 to 5,000. The weight average molecular weight of the resin can be measured by gel permeation chromatography (GPC) as a polystyrene-equivalent value.

[0230] -Polyvinyl acetal resin- Examples of polyvinyl acetal resins include polyvinyl formal resins and polyvinyl butyral resins, and polyvinyl butyral resins are preferred. Specific examples of polyvinyl acetal resins include S-LEC BH series, BX series (e.g., BX-5Z), KS series (e.g., KS-1), BL series, and BM series manufactured by Sekisui Chemical Co., Ltd.

[0231] -Acrylic resin- The acrylic resin refers to a polymer obtained by polymerizing a monomer component including a (meth)acrylic acid ester monomer. The monomer components constituting the acrylic resin may contain, in addition to the (meth)acrylic acid ester monomer, a (meth)acrylamide monomer, a styrene monomer, a functional group-containing monomer, or the like as copolymerization components. Specific examples of acrylic resins include "ARUFON UP-1000", "ARUFON UP-1010", "ARUFON UP-1020", "ARUFON UP-1021", "ARUFON UP-1061", "ARUFON UP-1080", "ARUFON UP-1110", "ARUFON UP-1170", "ARUFON UP-1190", "ARUFON UP-1500", "ARUFON UH-2000", "ARUFON UH-2041", "ARUFON UH-2190", "ARUFON UHA2012", "ARUFON UC-3510", "ARUFON UG-4010", "ARUFON US-6100", and "ARUFON US-6170", all manufactured by Toagosei Co., Ltd. These may be used alone or in combination of two or more.

[0232] -Polyolefin resin- Examples of polyolefin resins include ethylene-based copolymer resins such as low-density polyethylene, very low-density polyethylene, high-density polyethylene, ethylene-vinyl acetate copolymer, ethylene-ethyl acrylate copolymer, and ethylene-methyl acrylate copolymer; and polyolefin-based elastomers such as polypropylene and ethylene-propylene block copolymer.

[0233] -Polybutadiene resin- Examples of polybutadiene resins include hydrogenated polybutadiene skeleton-containing resins, hydroxy group-containing polybutadiene resins, phenolic hydroxy group-containing polybutadiene resins, carboxy group-containing polybutadiene resins, acid anhydride group-containing polybutadiene resins, epoxy group-containing polybutadiene resins, isocyanate group-containing polybutadiene resins, urethane group-containing polybutadiene resins, polyphenylene ether-polybutadiene resins, and the like.

[0234] -Polyamide-imide resin- Specific examples of polyamide-imide resins include "Viromax HR11NN" and "Viromax HR16NN" manufactured by Toyobo Co., Ltd. Specific examples of polyamide-imide resins also include modified polyamide-imides such as "KS9100" and "KS9300" (polysiloxane skeleton-containing polyamide-imide) manufactured by Hitachi Chemical Co., Ltd.

[0235] -Polyethersulfone resin- A specific example of the polyethersulfone resin is "PES5003P" manufactured by Sumitomo Chemical Co., Ltd.

[0236] -Polysulfone resin- Specific examples of polysulfone resins include polysulfones "P1700" and "P3500" manufactured by Solvay Advanced Polymers.

[0237] -Polyphenylene ether resin- A specific example of the polyphenylene ether resin is Noryl (registered trademark) SA90 manufactured by SABIC, etc. A specific example of the polyetherimide resin is Ultem manufactured by GE, etc.

[0238] -Polycarbonate resin- Examples of polycarbonate resins include hydroxyl group-containing carbonate resins, phenolic hydroxyl group-containing carbonate resins, carboxyl group-containing carbonate resins, acid anhydride group-containing carbonate resins, isocyanate group-containing carbonate resins, and urethane group-containing carbonate resins. Specific examples of polycarbonate resins include "FPC2136" manufactured by Mitsubishi Gas Chemical Company, Inc., "T6002" and "T6001" (polycarbonate diol) manufactured by Asahi Kasei Chemicals Corporation, and "C-1090", "C-2090", and "C-3090" (polycarbonate diol) manufactured by Kuraray Co., Ltd. Specific examples of polyether ether ketone resins include "Sumiploy K" manufactured by Sumitomo Chemical Co., Ltd. Examples of polyester resins include polyethylene terephthalate resins.

[0239] Unless otherwise specified, the weight average molecular weight of the thermoplastic resin is preferably 5,000 or more, more preferably 8,000 or more, even more preferably 10,000 or more, 15,000 or more, or 20,000 or more, and is preferably 200,000 or less, more preferably 150,000 or less, or 100,000 or less, even more preferably 80,000 or less, or 60,000 or less. The weight average molecular weight of the thermoplastic resin can be measured as a polystyrene-equivalent value by gel permeation chromatography (GPC).

[0240] When the resin composition of the present invention contains a thermoplastic resin, the content of the thermoplastic resin is preferably 0.1% by mass or more, more preferably 0.3% by mass or more, 0.5% by mass or more, 0.6% by mass or more, 0.8% by mass or more, or 1% by mass or more, when the resin component in the resin composition layer is 100% by mass. The upper limit of the content of the thermoplastic resin is not particularly limited, but is preferably 10% by mass or less, more preferably 8% by mass or less, and even more preferably 6% by mass or less, or 5% by mass or less.

[0241] <Thermosetting resin> The resin composition of the present invention may further contain a thermosetting resin, except for those corresponding to the radical polymerizable resin A.

[0242] Examples of the thermosetting resin include epoxy resins, phenolic resins, naphthol resins, benzoxazine resins, active ester resins, cyanate ester resins, carbodiimide resins, amine resins, acid anhydride resins, etc. The thermosetting resins may be used alone or in combination of two or more kinds in any ratio. Hereinafter, resins that can react with epoxy resins to cure the resin composition, such as phenol-based resins, naphthol-based resins, benzoxazine-based resins, active ester-based resins, cyanate ester-based resins, carbodiimide-based resins, amine-based resins, and acid anhydride-based resins, may be collectively referred to as "curing agents".

[0243] The type of epoxy resin is not particularly limited as long as it has one or more (preferably two or more) epoxy groups in one molecule. Examples of epoxy resins include bisphenol type epoxy resins, dicyclopentadiene type epoxy resins, trisphenol type epoxy resins, naphthol novolac type epoxy resins, phenol novolac type epoxy resins, tert-butyl-catechol type epoxy resins, naphthalene type epoxy resins, naphthol type epoxy resins, anthracene type epoxy resins, glycidylamine type epoxy resins, glycidyl ester type epoxy resins, cresol novolac type epoxy resins, biphenyl type epoxy resins, linear aliphatic epoxy resins, epoxy resins having a butadiene structure, alicyclic epoxy resins, heterocyclic epoxy resins, spiro ring-containing epoxy resins, cyclohexane type epoxy resins, cyclohexane dimethanol type epoxy resins, naphthylene ether type epoxy resins, trimethylol type epoxy resins, and tetraphenylethane type epoxy resins. Bisphenol type epoxy resin refers to an epoxy resin having a bisphenol structure, such as bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol S type epoxy resin, and bisphenol AF type epoxy resin. Biphenyl type epoxy resin refers to an epoxy resin having a biphenyl structure, where the biphenyl structure may have a substituent such as an alkyl group, an alkoxy group, or an aryl group. Therefore, bixylenol type epoxy resin and biphenyl aralkyl type epoxy resin are also included in biphenyl type epoxy resin.

[0244] Epoxy resins can be classified into epoxy resins that are liquid at a temperature of 20°C (hereinafter referred to as "liquid epoxy resins") and epoxy resins that are solid at a temperature of 20°C (hereinafter referred to as "solid epoxy resins"). 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.

[0245] The liquid epoxy resin is preferably a liquid epoxy resin having two or more epoxy groups in one molecule.

[0246] As the liquid epoxy resin, glycirol type epoxy resin, 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, phenol novolac type epoxy resin, alicyclic epoxy resin having an ester skeleton, cyclohexane dimethanol type epoxy resin, cyclic aliphatic glycidyl ether, and epoxy resin having a butadiene structure are preferred.

[0247] Specific examples of liquid epoxy resins include "EX-992L" manufactured by Nagase ChemteX Corporation, "YX7400" manufactured by Mitsubishi Chemical Corporation, "HP4032", "HP4032D", and "HP4032SS" (naphthalene type epoxy resins) manufactured by DIC Corporation; "828US", "828EL", and "825" (bisphenol A type epoxy resins) manufactured by Mitsubishi Chemical Corporation; "jER807" and "1750" (bisphenol F type epoxy resins) manufactured by Mitsubishi Chemical Corporation; "jER152" (phenol novolac type epoxy resin) manufactured by Ryo Chemical; "630", "630LSD", and "604" (glycidylamine type epoxy resin) manufactured by Mitsubishi Chemical; "ED-523T" (glycirol type epoxy resin) manufactured by ADEKA; "EP-3950L" and "EP-3980S" (glycidylamine type epoxy resin) manufactured by ADEKA; "EP-4088S" (dicyclopentadiene type epoxy resin) manufactured by ADEKA ); "ZX1059" manufactured by Nippon Steel Chemical & Material Co., Ltd. (a mixture of bisphenol A type epoxy resin and bisphenol F type epoxy resin); "EX-721" manufactured by Nagase ChemteX Corporation (glycidyl ester type epoxy resin); "EX-991L" manufactured by Nagase ChemteX Corporation (an epoxy resin containing an alkyleneoxy skeleton and a butadiene skeleton); "Celloxide 2021P" manufactured by Daicel Corporation (an alicyclic epoxy resin having an ester skeleton); "PB-3600" manufactured by Daicel Corporation, "JP-100" and "JP-200" manufactured by Nippon Soda Co., Ltd. (an epoxy resin having a butadiene structure); "ZX1658" and "ZX1658GS" manufactured by Nippon Steel Chemical & Material Co., Ltd. (liquid 1,4-glycidylcyclohexane type epoxy resin); "EG-280" manufactured by Osaka Gas Chemical Co., Ltd. (an epoxy resin containing a fluorene structure); and "EX-201" manufactured by Nagase ChemteX Corporation (cyclic aliphatic glycidyl ether).

[0248] As the solid epoxy resin, a solid epoxy resin having three or more epoxy groups in one molecule is preferable, and an aromatic solid epoxy resin having three or more epoxy groups in one molecule is more preferable.

[0249] Preferred solid epoxy resins include bixylenol type epoxy resins, naphthalene type epoxy resins, naphthalene type tetrafunctional epoxy resins, naphthol novolac type epoxy resins, cresol novolac type epoxy resins, dicyclopentadiene type epoxy resins, trisphenol type epoxy resins, naphthol type epoxy resins, biphenyl type epoxy resins, naphthylene ether type epoxy resins, anthracene type epoxy resins, bisphenol A type epoxy resins, bisphenol AF type epoxy resins, phenol aralkyl type epoxy resins, tetraphenylethane type epoxy resins, and phenolphthalimidine type epoxy resins.

[0250] Specific examples of solid epoxy resins include "HP4032H" (naphthalene type epoxy resin) manufactured by DIC Corporation; "HP-4700" and "HP-4710" (naphthalene type tetrafunctional epoxy resins) manufactured by DIC Corporation; "N-690" (cresol novolac type epoxy resin) manufactured by DIC Corporation; "N-695" (cresol novolac type epoxy resin) manufactured by DIC Corporation; "HP-7200", "HP-7200HH", "HP-7200H", and "HP-7200L" (dicyclopentadiene type epoxy resins) manufactured by DIC Corporation; "EXA-7311" and "E XA-7311-G3, EXA-7311-G4, EXA-7311-G4S, HP-6000, HP-6000L (naphthylene ether type epoxy resin); Nippon Kayaku's "EPPN-502H" (trisphenol type epoxy resin); Nippon Kayaku's "NC7000L" (naphthol novolac type epoxy resin); Nippon Kayaku's "NC3000H", "NC3000", "NC3000L", "NC3000FH", "NC3100" (biphenyl type epoxy resin); Nippon Steel Chemical & Material's "ESN475V" , "ESN4100V" (naphthalene type epoxy resin); "ESN485" (naphthol type epoxy resin) manufactured by Nippon Steel Chemical & Material Co., Ltd.; "ESN375" (dihydroxynaphthalene type epoxy resin) manufactured by Nippon Steel Chemical & Material Co., Ltd.; "YX4000H", "YX4000", "YX4000HK", "YL7890" (bixylenol type epoxy resin) manufactured by Mitsubishi Chemical Co., Ltd.; "YL6121" (biphenyl type epoxy resin) manufactured by Mitsubishi Chemical Co., Ltd.; "YX8800" (anthracene type epoxy resin) manufactured by Mitsubishi Chemical Co., Ltd. Examples of epoxy resins that can be used include "YX7700" (phenol aralkyl type epoxy resin) manufactured by Osaka Gas Chemicals; "PG-100" and "CG-500" manufactured by Osaka Gas Chemicals; "YL7760" (bisphenol AF type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "YL7800" (fluorene type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "jER1010" (bisphenol A type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "jER1031S" (tetraphenylethane type epoxy resin) manufactured by Mitsubishi Chemical Corporation; and "WHR991S" (phenolphthalimidine type epoxy resin) manufactured by Nippon Kayaku Co., Ltd.These may be used alone or in combination of two or more.

[0251] When a liquid epoxy resin and a solid epoxy resin are used in combination as the epoxy resin, the mass ratio thereof (liquid epoxy resin:solid epoxy resin) is preferably 10:1 to 1:50, more preferably 5:1 to 1:20, even more preferably 2:1 to 1:10, and particularly preferably 1:1 to 1:3.

[0252] The epoxy equivalent of the epoxy resin is preferably 50 g / eq. to 5,000 g / eq., more preferably 60 g / eq. to 2,000 g / eq., even more preferably 70 g / eq. to 1,000 g / eq., and even more preferably 80 g / eq. to 500 g / eq. The epoxy equivalent is the mass of the resin per equivalent of epoxy group. This epoxy equivalent can be measured according to JIS K7236.

[0253] The weight average molecular weight of the epoxy resin is preferably 100 to 5,000, more preferably 250 to 3,000, and further preferably 400 to 1500. The weight average molecular weight of the resin can be measured by gel permeation chromatography (GPC) as a polystyrene-equivalent value.

[0254] When the resin composition of the present invention contains an epoxy resin as a thermosetting resin, the content of the epoxy resin is not particularly limited, but is preferably 5% by mass or more, more preferably 10% by mass or more, and even more preferably 12% by mass or more, 14% by mass or more, or 15% by mass or more, when the resin component in the resin composition is 100% by mass. The upper limit of the content is not particularly limited and may be determined depending on the properties required of the resin composition, but may be, for example, 60% by mass or less, 50% by mass or less, or 40% by mass or less.

[0255] As the active ester resin as the thermosetting resin, a compound having one or more active ester groups in one molecule can be used. Among them, as the active ester resin, a compound having two or more highly reactive ester groups in one molecule, such as phenol esters, thiophenol esters, N-hydroxyamine esters, and esters of heterocyclic hydroxy compounds, is preferable. The active ester resin is preferably one 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 resin derived from a carboxylic acid compound is preferable, an active ester resin obtained from a carboxylic acid compound and a hydroxy compound is more preferable, and an active ester resin obtained from a carboxylic acid compound and an aromatic hydroxy compound is even more preferable.

[0256] The carboxylic acid compound may be either an aromatic carboxylic acid compound or an aliphatic carboxylic acid compound, and examples thereof include benzoic acid, acetic acid, succinic acid, maleic acid, itaconic acid, phthalic acid, isophthalic acid, terephthalic acid, pyromellitic acid, and halides thereof.

[0257] Examples of aromatic hydroxy compounds include (i) polyaddition products of unsaturated aliphatic cyclic compounds containing two double bonds in one molecule and phenols, (ii) various bisphenol compounds, (iii) aromatic polyols having two or more hydroxyl groups bonded to the carbon atoms on the aromatic ring, and (iv) aromatic monools having one hydroxyl group bonded to the carbon atoms on the aromatic ring. Examples of polyaddition products of unsaturated aliphatic cyclic compounds and phenols include polyaddition products of unsaturated aliphatic cyclic compounds such as dicyclopentadiene, tetrahydroindene, norbornadiene, limonene, and vinylcyclohexene with phenols that may have a substituent (e.g., phenol, cresol, xylenol, ethylphenol, propylphenol, vinylphenol, allylphenol, phenylphenol, benzylphenol, halophenol, etc.), and specifically, for example, dicyclopentadiene-phenols polyaddition products. Examples of bisphenol compounds include bisphenol A, bisphenol F, bisphenol AF, bisphenol AP, bisphenol B, bisphenol BP, bisphenol C, and bisphenol M. Examples of aromatic polyols having two or more hydroxy groups bonded to carbon atoms on an aromatic ring include hydroquinone, resorcinol, catechol, 1,5-dihydroxynaphthalene, 1,6-dihydroxynaphthalene, 2,6-dihydroxynaphthalene, dihydroxybenzophenone, trihydroxybenzophenone, tetrahydroxybenzophenone, phloroglucinol, benzenetriol, and phenol novolak. Examples of aromatic monools having one hydroxy group bonded to a carbon atom on an aromatic ring include phenol, cresol, xylenol, ethylphenol, propylphenol, vinylphenol, allylphenol, phenylphenol, benzylphenol, halophenol, naphthol, methylnaphthol, dimethylnaphthol, ethylnaphthol, propylnaphthol, vinylnaphthol, allylnaphthol, phenylnaphthol, benzylnaphthol, and halonaphthol.

[0258] Preferred specific examples of the active ester resin include active ester resins containing a dicyclopentadiene-type diphenol structure, active ester resins containing a naphthalene structure, active ester resins containing an acetylated product of phenol novolac, and active ester resins containing a benzoylated product of phenol novolac. Among them, active ester resins containing a naphthalene structure and active ester resins containing a dicyclopentadiene-type diphenol structure are more preferred. The "dicyclopentadiene-type diphenol structure" refers to a divalent structural unit consisting of phenylene-dicyclopentylene-phenylene.

[0259] Commercially available active ester resins include active ester resins containing a dicyclopentadiene-type diphenol structure, such as "EXB9451", "EXB9460", "EXB9460S", "HPC-8000-65T", "HPC-8000H-65TM", and "EXB-8000L-65TM" (manufactured by DIC Corporation); active ester resins containing a naphthalene structure, such as "EXB9416-70BK", "EXB-8100L-65T", "EXB-8150L-65T", "EXB-8150-65T", "HPC-8150-60T", and "HPC-8150-62T" (manufactured by DIC Corporation); and phenol novo Examples of active ester resins containing acetylated phenol novolac include "DC808" (manufactured by Mitsubishi Chemical Corporation); examples of active ester resins containing benzoylated phenol novolac include "YLH1026" (manufactured by Mitsubishi Chemical Corporation); examples of active ester resins which are acetylated phenol novolac include "DC808" (manufactured by Mitsubishi Chemical Corporation); examples of active ester resins which are benzoylated phenol novolac include "YLH1026" (manufactured by Mitsubishi Chemical Corporation), "YLH1030" (manufactured by Mitsubishi Chemical Corporation), "YLH1048" (manufactured by Mitsubishi Chemical Corporation); and "EXB-8500-65T" (manufactured by DIC Corporation).

[0260] As the phenolic resin and naphtholic resin as the thermosetting resin, those having a novolac structure are preferred from the viewpoint of heat resistance and water resistance. Also, from the viewpoint of adhesion to the conductor layer, nitrogen-containing phenolic curing agents and nitrogen-containing naphtholic resins are preferred, and triazine skeleton-containing phenolic resins and triazine skeleton-containing naphtholic resins are more preferred.

[0261] Specific examples of phenol-based resins and naphthol-based resins include "MEH-7700", "MEH-7810", and "MEH-7851" manufactured by Meiwa Chemical Industry Co., Ltd.; "NHN", "CBN", and "GPH" manufactured by Nippon Kayaku Co., Ltd.; "SN170", "SN180", "SN190", "SN475", "SN485", "SN495", "SN-495V", "SN375", and "SN395" manufactured by Nippon Steel Chemical & Material Co., Ltd.; and "TD-2090", "LA-7052", "LA-7054", "LA-1356", "LA-3018-50P", and "EXB-9500" manufactured by DIC Corporation.

[0262] Specific examples of benzoxazine-based resins as thermosetting resins include "JBZ-OD100" (benzoxazine ring equivalent: 218), "JBZ-OP100D" (benzoxazine ring equivalent: 218), and "ODA-BOZ" (benzoxazine ring equivalent: 218) manufactured by JFE Chemical Corporation; "Pd" (benzoxazine ring equivalent: 217) and "Fa" (benzoxazine ring equivalent: 217) manufactured by Shikoku Chemical Industry Co., Ltd.; and "HFB2006M" (benzoxazine ring equivalent: 432) manufactured by Showa Polymer Co., Ltd.

[0263] Examples of cyanate ester resins as thermosetting resins include bifunctional cyanate resins such as bisphenol A dicyanate, polyphenol cyanate, oligo(3-methylene-1,5-phenylene cyanate), 4,4'-methylenebis(2,6-dimethylphenyl cyanate), 4,4'-ethylidene diphenyl dicyanate, hexafluorobisphenol A dicyanate, 2,2-bis(4-cyanate)phenylpropane, 1,1-bis(4-cyanate phenylmethane), bis(4-cyanate-3,5-dimethylphenyl)methane, 1,3-bis(4-cyanate phenyl-1-(methylethylidene))benzene, bis(4-cyanate phenyl)thioether, and bis(4-cyanate phenyl)ether; polyfunctional cyanate resins derived from phenol novolac and cresol novolac; and prepolymers in which these cyanate resins are partially converted to triazine. Specific examples of cyanate ester resins include "PT30", "PT30S" and "PT60" (phenol novolac type multifunctional cyanate ester resins), "ULL-950S" (multifunctional cyanate ester resin), "BA230" and "BA230S75" (prepolymers in which part or all of bisphenol A dicyanate has been converted to triazine to form a trimer), all of which are manufactured by Lonza Japan.

[0264] Specific examples of carbodiimide-based resins as thermosetting resins include Carbodilite (registered trademark) V-03 (carbodiimide group equivalent: 216, V-05 (carbodiimide group equivalent: 216), V-07 (carbodiimide group equivalent: 200); V-09 (carbodiimide group equivalent: 200), all manufactured by Nisshinbo Chemical Inc.; and Stavaxol (registered trademark) P (carbodiimide group equivalent: 302), all manufactured by Rhein Chemie.

[0265] The amine-based resin as the thermosetting resin may be a resin having one or more amino groups in one molecule, such as aliphatic amines, polyether amines, alicyclic amines, aromatic amines, etc., and among them, aromatic amines are preferred from the viewpoint of achieving the desired effects of the present invention. The amine-based resin is preferably a primary amine or secondary amine, and more preferably a primary amine. Specific examples of amine resins include 4,4'-methylenebis(2,6-dimethylaniline), diphenyldiaminosulfone, 4,4'-diaminodiphenylmethane, 4,4'-diaminodiphenylsulfone, 3,3'-diaminodiphenylsulfone, m-phenylenediamine, m-xylylenediamine, diethyltoluenediamine, 4,4'-diaminodiphenylether, 3,3'-dimethyl-4,4'-diaminobiphenyl, 2,2'-dimethyl-4,4'-diaminobiphenyl, 3,3'-dihydroxybenzidine, 2,2-bis(3-amino-4-hydroxyphenyl)-2,2'-diphenylpropanediamine, 2,2' ... phenyl)propane, 3,3-dimethyl-5,5-diethyl-4,4-diphenylmethanediamine, 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, etc. As the amine-based resin, commercially available products may be used, for example, "KAYABOND C-200S", "KAYABOND C-100", "KAYAHARD AA", "KAYAHARD AB", "KAYAHARD AS" manufactured by Nippon Kayaku Co., Ltd., and "Epicure W" manufactured by Mitsubishi Chemical Corporation.

[0266] Examples of acid anhydride resins as thermosetting resins include resins having one or more acid anhydride groups in one molecule. Specific examples of acid anhydride resins include phthalic anhydride, tetrahydrophthalic anhydride, hexahydrophthalic anhydride, methyltetrahydrophthalic anhydride, methylhexahydrophthalic anhydride, methylnadic anhydride, hydrogenated methylnadic anhydride, trialkyltetrahydrophthalic anhydride, dodecenyl succinic anhydride, 5-(2,5-dioxotetrahydro-3-furanyl)-3-methyl-3-cyclohexene-1,2-dicarboxylic anhydride, trimellitic anhydride, pyromellitic anhydride, and benzophenonetetracarboxylic dianhydride. Examples of acid anhydrides include anhydrides, 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), and polymeric acid anhydrides such as styrene-maleic acid resin, which is a copolymer of styrene and maleic acid.

[0267] When the resin composition of the present invention contains a thermosetting resin (particularly an epoxy resin), the content of the curing agent that the resin composition of the present invention may contain is preferably 1 mass% or more, more preferably 5 mass% or more, and even more preferably 10 mass% or more, relative to 100 mass% of the resin component in the resin composition, and is preferably 30 mass% or less, more preferably 25 mass% or less, and even more preferably 20 mass% or less.

[0268] <Curing accelerator> The resin composition of the present invention may further contain a curing accelerator as an optional component. By including a curing accelerator, it becomes possible to further accelerate polymerization by heat.

[0269] Examples of the curing accelerator include phosphorus-based curing accelerators, amine-based curing accelerators, imidazole-based curing accelerators, guanidine-based curing accelerators, metal-based curing accelerators, peroxide-based curing accelerators, etc. The curing accelerators may be used alone or in combination of two or more.

[0270] When the resin composition of the present invention contains a thermosetting resin, the content of the curing accelerator in the resin composition is preferably 0.1 mass% or more, more preferably 0.3 mass% or more or 0.5 mass% or more, when the resin component in the resin composition is 100 mass%, and the upper limit is preferably 4 mass% or less, more preferably 3 mass% or less.

[0271] <Other additives> The resin composition of the present invention may further contain other additives as optional components in addition to the above-mentioned components.Such additives include, for example, radical polymerization initiators such as peroxide radical polymerization initiators and azo radical polymerization initiators; organic metal compounds such as organic copper compounds, organic zinc compounds, and organic cobalt compounds; colorants such as phthalocyanine blue, phthalocyanine green, iodine green, diazo yellow, crystal violet, titanium oxide, and carbon black; polymerization inhibitors such as hydroquinone, catechol, pyrogallol, and phenothiazine; leveling agents such as silicone leveling agents and acrylic polymer leveling agents; thickeners such as bentone and montmorillonite; defoamers such as silicone defoamers, acrylic defoamers, fluorine defoamers, and vinyl resin defoamers; ultraviolet absorbers such as benzotriazole ultraviolet absorbers; adhesion improvers such as urea silane; triazole adhesion imparting agents, tetrazole adhesion inhibitors Adhesion imparting agents, adhesion imparting agents such as triazine adhesion imparting agents; antioxidants such as hindered phenol antioxidants; fluorescent brighteners such as stilbene derivatives; surfactants such as fluorine-based surfactants and silicone-based surfactants; flame retardants such as phosphorus-based flame retardants (e.g., phosphate ester compounds, phosphazene compounds, phosphinic acid compounds, red phosphorus), nitrogen-based flame retardants (e.g., melamine sulfate), halogen-based flame retardants, and inorganic flame retardants (e.g., antimony trioxide); dispersants such as phosphate ester dispersants, polyoxyalkylene dispersants, acetylene dispersants, silicone-based dispersants, anionic dispersants, and cationic dispersants; stabilizers such as borate-based stabilizers, titanate-based stabilizers, aluminate-based stabilizers, zirconate-based stabilizers, isocyanate-based stabilizers, carboxylic acid-based stabilizers, and carboxylic anhydride-based stabilizers, and chelate fluxing agents. The content of such additives may be determined according to the properties required for the thermosetting resin composition. It is preferable that the resin composition of the present invention substantially does not contain a photopolymerization initiator such as a photoacid generator or a photoradical generator (more specifically, when the resin component in the resin composition is taken as 100% by mass, the content is less than 0.1% by mass, 0.05% by mass or less, 0.04% by mass or less, 0.02% by mass or less, 0.01% by mass or less, less than 0.01% by mass, 0.005% by mass or less, 0.001% by mass or less, or less than 0.001% by mass).In addition, it is preferable that the resin composition of the present invention is substantially free of a chelating flux agent (more specifically, when the resin component in the resin composition is taken as 100 mass%, the content of the chelating flux agent is less than 0.1 mass%, 0.05 mass% or less, 0.04 mass% or less, 0.02 mass% or less, or 0.01 mass% or less).

[0272] <Organic solvent> The thermosetting resin composition of the present invention may further contain an organic solvent as a volatile component. Examples of the organic solvent include ketone-based solvents such as acetone, methyl ethyl ketone, methyl isobutyl ketone, and cyclohexanone; ester-based solvents such as methyl acetate, ethyl acetate, butyl acetate, isobutyl acetate, isoamyl acetate, methyl propionate, ethyl propionate, and γ-butyrolactone; ether-based solvents such as tetrahydropyran, tetrahydrofuran, 1,4-dioxane, diethyl ether, diisopropyl ether, dibutyl ether, and diphenyl ether; alcohol-based solvents such as methanol, ethanol, propanol, butanol, and ethylene glycol; 2-ethoxyethyl acetate, propylene glycol monomethyl ether acetate, diethylene glycol monoethyl ether acetate, ethyl diglycol acetate, γ-butyrolactone, and methyl methoxypropionate. Examples of the organic solvent include ether ester solvents such as ethyl lactate, ethyl lactate, and methyl 2-hydroxyisobutyrate; ether alcohol solvents such as 2-methoxypropanol, 2-methoxyethanol, 2-ethoxyethanol, propylene glycol monomethyl ether, and diethylene glycol monobutyl ether (butyl carbitol); amide solvents such as N,N-dimethylformamide, N,N-dimethylacetamide, and N-methyl-2-pyrrolidone; sulfoxide solvents such as dimethyl sulfoxide; nitrile solvents such as acetonitrile and propionitrile; aliphatic hydrocarbon solvents such as hexane, cyclopentane, cyclohexane, and methylcyclohexane; and aromatic hydrocarbon solvents such as benzene, toluene, xylene, ethylbenzene, and trimethylbenzene. The organic solvent may be used alone or in combination of two or more.

[0273] The resin composition of the present invention can be produced, for example, by adding and mixing the radical polymerizable resin A, di-t-amyl peroxide, and, if necessary, the inorganic filler, the thermoplastic resin, the thermosetting resin, the curing accelerator, other additives, and the organic solvent in any order and / or all at once in any preparation vessel. In addition, the temperature can be appropriately set during the process of adding and mixing each component, and heating and / or cooling may be performed temporarily or throughout. In addition, during or after the process of adding and mixing, the resin composition may be stirred or shaken using a stirring device or shaking device such as a mixer to disperse it uniformly. In addition, degassing may be performed under low pressure conditions such as under vacuum at the same time as stirring or shaking.

[0274] <Physical properties and applications of resin compositions> The resin composition of the present invention contains a radical polymerizable resin A and di-t-amyl peroxide, which makes it possible to obtain a cured product that exhibits excellent resin flatness, good dielectric properties, and peel strength.

[0275] The resin composition of the present invention exhibits the property of producing a cured product (insulating layer) with excellent resin flatness. Specifically, when an insulating layer is formed on an inner layer substrate (inner layer circuit thickness 18 μm, comb pattern with L / S=175 / 175 μm) using the resin composition according to the method described later in <Test Example 3: Measurement of resin flatness>, the difference between the maximum height and the minimum height of the surface of the insulating layer can be suppressed to less than 2 μm.

[0276] The resin composition of the present invention exhibits the property of producing a cured product (insulating layer) with a low dielectric constant. For example, when the resin composition is thermally cured at 190°C for 90 minutes according to the method described later in <Test Example 2: Measurement of Dielectric Properties (Dielectric Constant, Dielectric Loss Tangent)> to form a cured product, the dielectric constant of the cured product measured at 5.8 GHz and 23°C is preferably 3.5 or less, more preferably 3.4 or less, even more preferably 3.3 or less, or 3.2 or less.

[0277] The resin composition of the present invention exhibits the property of producing a cured product (insulating layer) with a low dielectric loss tangent. For example, when the resin composition is thermally cured at 190°C for 90 minutes according to the method described later in <Test Example 2: Measurement of Dielectric Properties (Dielectric Constant, Dielectric Loss Tangent)> to form a cured product, the dielectric loss tangent of the cured product measured at 5.8 GHz and 23°C is preferably 0.005 or less, more preferably 0.004 or less, even more preferably 0.003 or less, 0.0028 or less, 0.0026 or less, 0.0025 or less, or 0.0024 or less.

[0278] The resin composition of the present invention exhibits the property of providing a cured product (insulating layer) with high peel strength between the resin composition and a conductor layer. For example, when the peel strength between the resin composition and a copper foil is measured according to the method described later in <Test Example 4: Measurement of Peel Strength of Copper Foil>, the peel strength of the cured product of the resin composition of the present invention is preferably 0.5 kgf / cm or more, more preferably 0.6 kgf / cm or more, further preferably 0.62 kgf / cm or more, 0.64 kgf / cm or more, or 0.65 kgf / cm or more.

[0279] The resin composition of the present invention can provide a cured product having excellent resin flatness, good dielectric properties and peel strength. Therefore, the resin composition of the present invention can be suitably used as a resin composition for forming an insulating layer of a printed wiring board (resin composition for insulating layer of printed wiring board), and more suitably used as a resin composition for forming an interlayer insulating layer of a printed wiring board (resin composition for interlayer insulating layer of printed wiring board). The resin composition of the present invention can also be suitably used when the printed wiring board is a circuit board with built-in components. The resin composition of the present invention can also be suitably used as a resin composition for forming an insulating layer of a rewiring board of a semiconductor package (resin composition for insulating layer of rewiring board). In the present invention, the printed wiring board and the rewiring board are collectively referred to as "circuit board", and therefore the resin composition of the present invention can be suitably used for the insulating layer of a circuit board.

[0280] The resin composition of the present invention can also be used in a wide range of applications requiring a resin composition, such as sheet-like laminate materials such as resin sheets and prepregs, solder resists, die bonding materials, hole filling resins, sealing resins, and component embedding resins.

[0281] [Sheet-type laminated materials (resin sheets, prepregs)] The resin composition of the present invention can be used as it is, but it may also be used in the form of a sheet-like laminate material containing the resin composition.

[0282] As the sheet-like laminate material, the following resin sheets and prepregs are preferred.

[0283] In one embodiment, the resin sheet includes a support and a layer of a resin composition (hereinafter simply referred to as a "resin composition layer") provided on the support, and is characterized in that the resin composition layer is formed from the resin composition of the present invention.

[0284] The thickness of the resin composition layer may vary depending on the application, and may be appropriately determined depending on the application. For example, the thickness of the resin composition layer is preferably 120 μm or less, 100 μm or less, 80 μm or less, 60 μm or less, 50 μm or less, 40 μm or less, or 30 μm or less from the viewpoint of thinning the printed wiring board or semiconductor package. The lower limit of the thickness of the resin composition layer is not particularly limited, but may usually be 1 μm or more, 5 μm or more, etc.

[0285] Examples of the support include a thermoplastic resin film, a metal foil, and a release paper, and a thermoplastic resin film and a metal foil are preferred. Thus, in a preferred embodiment, the support is a thermoplastic resin film or a metal foil.

[0286] When a thermoplastic resin film is used as the support, examples of the thermoplastic resin include polyesters such as polyethylene terephthalate (PET) and polyethylene naphthalate (PEN), acrylics such as polycarbonate (PC) and polymethyl methacrylate (PMMA), cyclic polyolefins, triacetyl cellulose (TAC), polyether sulfide (PES), polyether ketone, polyimide, etc. Among these, polyethylene terephthalate and polyethylene naphthalate are preferred, and inexpensive polyethylene terephthalate is particularly preferred.

[0287] When a metal foil is used as the support, examples of the metal foil include copper foil, aluminum foil, etc., and copper foil is preferred. As the copper foil, a foil made of a single metal, copper, or an alloy of copper and another metal (e.g., tin, chromium, silver, magnesium, nickel, zirconium, silicon, titanium, etc.) may be used.

[0288] The support may be subjected to a matte treatment, a corona treatment, or an antistatic treatment on the surface to be bonded to the resin composition layer. In addition, a support with a release layer having a release layer on the surface to be bonded to the resin composition layer may be used as the support. The release agent used in the release layer of the support with a release layer may be, for example, one or more release agents selected from the group consisting of alkyd resins, polyolefin resins, urethane resins, and silicone resins. The support with a release layer may be a commercially available product, for example, "SK-1", "AL-5", and "AL-7" manufactured by Lintec Corporation, "Lumirror T60" manufactured by Toray Industries, Inc., "Purex" manufactured by Teijin Limited, and "Unipeel" manufactured by Unitika Limited, which are PET films having a release layer mainly composed of an alkyd resin-based release agent.

[0289] The thickness of the support is not particularly limited, but is preferably in the range of 5 μm to 75 μm, and more preferably in the range of 10 μm to 60 μm. When a support with a release layer is used, it is preferable that the total thickness of the support with a release layer is in the above range.

[0290] When a metal foil is used as the support, a metal foil with a support substrate may be used, which is a thin metal foil with a peelable support substrate attached thereto. In one embodiment, the metal foil with a support substrate includes a support substrate, a release layer provided on the support substrate, and a metal foil provided on the release layer. When a metal foil with a support substrate is used as the support, the resin composition layer is provided on the metal foil.

[0291] In the metal foil with a supporting substrate, the material of the supporting substrate is not particularly limited, and examples thereof include copper foil, aluminum foil, stainless steel foil, titanium foil, copper alloy foil, etc. When copper foil is used as the supporting substrate, it may be electrolytic copper foil or rolled copper foil. In addition, the release layer is not particularly limited as long as it can release the metal foil from the supporting substrate, and examples thereof include an alloy layer of an element selected from the group consisting of Cr, Ni, Co, Fe, Mo, Ti, W, and P; an organic coating, etc.

[0292] In the metal foil with a supporting substrate, the material of the metal foil is preferably, for example, copper foil or copper alloy foil.

[0293] In the metal foil with a supporting substrate, the thickness of the supporting substrate is not particularly limited, but is preferably in the range of 10 μm to 150 μm, more preferably in the range of 10 μm to 100 μm, and the thickness of the metal foil may be, for example, in the range of 0.1 μm to 10 μm.

[0294] In one embodiment, the resin sheet may further include an optional layer as necessary. For example, such an optional layer may be a protective film provided on the surface of the resin composition layer that is not bonded to the support (i.e., the surface opposite to the support). The thickness of the protective film is not particularly limited, but is, for example, 1 μm to 40 μm. By laminating the protective film, it is possible to suppress adhesion of dirt and the like to the surface of the resin composition layer and scratches.

[0295] The resin sheet can be produced, for example, by preparing a liquid resin composition as is or a resin varnish by dissolving the resin composition in an organic solvent, applying this onto a support using a die coater or the like, and then drying to form a resin composition layer.

[0296] The organic solvent may be the same as the organic solvent described as a component of the resin composition. The organic solvent may be used alone or in combination of two or more kinds.

[0297] Drying may be performed by a known method such as heating or hot air blowing. Drying conditions are not particularly limited, but drying is performed so that the content of the organic solvent in the resin composition layer becomes 10% by mass or less, preferably 5% by mass or less. Although it varies depending on the boiling point of the organic solvent in the resin composition or resin varnish, for example, when a resin composition or resin varnish containing 30% by mass to 60% by mass of the organic solvent is used, the resin composition layer can be formed by drying at 50°C to 150°C for 3 minutes to 10 minutes.

[0298] The resin sheet can be stored in a rolled state. When the resin sheet has a protective film, it can be used by peeling off the protective film.

[0299] In one embodiment, the prepreg is formed by impregnating a sheet-like fiber substrate with the resin composition of the present invention.

[0300] The sheet-like fiber substrate used for the prepreg is not particularly limited, and can be a substrate commonly used for prepreg, such as glass cloth, aramid nonwoven fabric, or liquid crystal polymer nonwoven fabric. From the viewpoint of thinning of printed wiring boards and semiconductor chip packages, the thickness of the sheet-like fiber substrate is preferably 50 μm or less, more preferably 40 μm or less, even more preferably 30 μm or less, and particularly preferably 20 μm or less. The lower limit of the thickness of the sheet-like fiber substrate is not particularly limited. It is usually 10 μm or more.

[0301] The prepreg can be produced by a known method such as a hot melt method or a solvent method.

[0302] The thickness of the prepreg may be in the same range as that of the resin composition layer in the above-mentioned resin sheet.

[0303] The sheet-like laminate material of the present invention can be suitably used to form an insulating layer of a printed wiring board (for the insulating layer of a printed wiring board), and can be more suitably used to form an interlayer insulating layer of a printed wiring board (for the insulating layer of a printed wiring board). The sheet-like laminate material of the present invention can also be suitably used to form an insulating layer of a rewiring board of a semiconductor package (for the insulating layer of a rewiring board). That is, the sheet-like laminate material of the present invention can be suitably used as an insulating layer of a circuit board.

[0304] [Circuit board] The resin composition of the present invention can be used to form an insulating layer for a circuit board. The present invention also provides such a circuit board, i.e., a circuit board including an insulating layer made of a cured product of the resin composition of the present invention.

[0305] <Printed wiring board> In one embodiment, the circuit board of the present invention is a printed wiring board.

[0306] The printed wiring board can be produced, for example, by using the above-mentioned resin sheet, by a method including the following steps (I) and (II). (I) A step of laminating a resin sheet on an inner layer substrate such that a resin composition layer of the resin sheet is bonded to the inner layer substrate. (II) A step of curing (e.g., heat curing) the resin composition layer to form an insulating layer.

[0307] The "inner layer substrate" used in step (I) is a member that becomes the substrate of the printed wiring board, and examples thereof include a glass epoxy substrate, a metal substrate, a polyester substrate, a polyimide substrate, a BT resin substrate, and a thermosetting polyphenylene ether substrate. The substrate may have a conductor layer on one or both sides, and the conductor layer may be patterned. An inner layer substrate having a conductor layer (circuit) formed on one or both sides of the substrate may be called an "inner layer circuit substrate". In addition, an intermediate product on which an insulating layer and / or a conductor layer is to be formed during the manufacture of a printed wiring board is also included in the "inner layer substrate" of the present invention. When the printed wiring board is a circuit board with built-in components, an inner layer substrate with built-in components may be used.

[0308] The lamination of the inner layer substrate and the resin sheet can be carried out, for example, by thermocompression bonding the resin sheet to the inner layer substrate from the support side. Examples of the member for thermocompression bonding the resin sheet to the inner layer substrate (hereinafter also referred to as the "thermocompression bonding member") include a heated metal plate (such as a SUS plate) or a metal roll (SUS roll). The thermocompression bonding member may be pressed directly onto the resin sheet, or may be pressed via an elastic material such as heat-resistant rubber so that the resin sheet can sufficiently follow the surface irregularities of the inner layer substrate.

[0309] The lamination of the inner layer substrate and the resin sheet may be performed by a vacuum lamination method. In the vacuum lamination method, the thermocompression temperature is preferably in the range of 60°C to 160°C, more preferably in the range of 80°C to 140°C, the thermocompression pressure is preferably in the range of 0.098MPa to 1.77MPa, more preferably in the range of 0.29MPa to 1.47MPa, and the thermocompression time is preferably in the range of 20 seconds to 400 seconds, more preferably in the range of 30 seconds to 300 seconds. The lamination may be performed under reduced pressure conditions, preferably at a pressure of 26.7hPa or less.

[0310] The lamination can be performed by a commercially available vacuum laminator, such as a vacuum pressure laminator manufactured by Meiki Seisakusho Co., Ltd., a vacuum applicator manufactured by Nikko Materials Co., Ltd., or a batch type vacuum pressure laminator.

[0311] After lamination, the laminated resin sheet may be smoothed under normal pressure (atmospheric pressure), for example, by pressing a thermocompression member from the support side. The pressing conditions for the smoothing treatment may be the same as the thermocompression conditions for the lamination. The smoothing treatment may be performed using a commercially available laminator. The lamination and smoothing treatment may be performed consecutively using the commercially available vacuum laminator.

[0312] The support may be removed between step (I) and step (II), or after step (II). When a metal foil is used as the support, the conductor layer may be formed using the metal foil without peeling off the support. When a metal foil with a support substrate is used as the support, the support substrate (and the peel layer) may be peeled off. Then, the conductor layer can be formed using the metal foil.

[0313] In step (II), the resin composition layer is cured (for example, thermally cured) to form an insulating layer made of a cured product of the resin composition. The curing conditions for the resin composition layer are not particularly limited, and conditions that are usually adopted when forming an insulating layer for a printed wiring board may be used.

[0314] For example, the thermal curing conditions for the resin composition layer vary depending on the type of resin composition, etc., but in one embodiment, the curing temperature is preferably 140° C. to 250° C., more preferably 150° C. to 240° C., and even more preferably 170° C. to 230° C. The curing time can be preferably 5 minutes to 240 minutes, more preferably 10 minutes to 150 minutes, and even more preferably 15 minutes to 120 minutes.

[0315] Before the resin composition layer is thermally cured, the resin composition layer may be preheated at a temperature lower than the curing temperature. For example, prior to thermally curing the resin composition layer, the resin composition layer may be preheated at a temperature of 50° C. to 140° C., preferably 60° C. to 135° C., more preferably 70° C. to 130° C. for 5 minutes or more, preferably 5 minutes to 150 minutes, more preferably 15 minutes to 120 minutes, and even more preferably 15 minutes to 100 minutes.

[0316] In manufacturing a printed wiring board, the steps of (III) drilling holes in the insulating layer, (IV) roughening the insulating layer, and (V) forming a conductor layer may be further carried out. These steps (III) to (V) may be carried out according to various methods known to those skilled in the art that are used in manufacturing printed wiring boards. When the support is removed after step (II), the removal of the support may be carried out between step (II) and step (III), between step (III) and step (IV), or between step (IV) and step (V). In addition, the formation of the insulating layer and the conductor layer in steps (I) to (V) may be repeated to form a multilayer wiring board, as necessary.

[0317] In another embodiment, the printed wiring board of the present invention can be manufactured using the above-mentioned prepreg. The manufacturing method is basically the same as when a resin sheet is used.

[0318] Step (III) is a step of drilling holes in the insulating layer, which allows holes such as via holes and through holes to be formed in the insulating layer. Step (III) may be performed using, for example, a drill, a laser, plasma, etc., depending on the composition of the resin composition used to form the insulating layer. The dimensions and shape of the holes may be appropriately determined depending on the design of the printed wiring board.

[0319] Step (IV) is a step of roughening the insulating layer. Usually, in this step (IV), smear removal (desmear) is also performed. The procedure and conditions of the roughening treatment are not particularly limited, and known procedures and conditions that are usually used when forming an insulating layer of a printed wiring board can be adopted. For example, the insulating layer can be roughened by performing a swelling treatment with a swelling liquid, a roughening treatment with an oxidizing agent, and a neutralization treatment with a neutralizing liquid in this order.

[0320] The swelling liquid used in the roughening treatment is not particularly limited, but includes an alkaline solution, a surfactant solution, etc., and is preferably an alkaline solution, and more preferably a sodium hydroxide solution or a potassium hydroxide solution. Examples of commercially available swelling liquids include "Swelling Dip Securigans P" and "Swelling Dip Securigans SBU" manufactured by Atotech Japan. The swelling treatment using the swelling liquid is not particularly limited, but can be performed by immersing the insulating layer in a swelling liquid at 30°C to 90°C for 1 to 20 minutes, for example. From the viewpoint of suppressing the swelling of the resin of the insulating layer to an appropriate level, it is preferable to immerse the insulating layer in a swelling liquid at 40°C to 80°C for 5 to 15 minutes.

[0321] The oxidizing agent used in the roughening treatment is not particularly limited, but examples thereof include an alkaline permanganate solution in which potassium permanganate or sodium permanganate is dissolved in an aqueous solution of sodium hydroxide. The roughening treatment using an oxidizing agent such as an alkaline permanganate solution is preferably performed by immersing the insulating layer in an oxidizing agent solution heated to 60°C to 100°C for 10 minutes to 30 minutes. The concentration of permanganate in the alkaline permanganate solution is preferably 5% by mass to 10% by mass. Examples of commercially available oxidizing agents include alkaline permanganate solutions such as "Concentrate Compact CP" and "Dosing Solution Securigans P" manufactured by Atotech Japan.

[0322] The neutralizing solution used in the roughening treatment is preferably an acidic aqueous solution, and a commercially available product such as "Reduction Solution Securigant P" manufactured by Atotech Japan can be mentioned.

[0323] The treatment with the neutralizing solution can be carried out by immersing the surface that has been roughened with an oxidizing agent in a neutralizing solution at 30° C. to 80° C. for 5 to 30 minutes. From the viewpoint of workability, etc., a method in which the object that has been roughened with an oxidizing agent is immersed in a neutralizing solution at 40° C. to 70° C. for 5 to 20 minutes is preferred.

[0324] Step (V) is a step of forming a conductor layer, and the conductor layer is formed on the insulating layer. The conductor material used for the conductor layer is not particularly limited. In a preferred embodiment, the conductor layer contains one or more metals selected from the group consisting of gold, platinum, palladium, silver, copper, aluminum, cobalt, chromium, zinc, nickel, titanium, tungsten, iron, tin and indium. The conductor layer may be a single metal layer or an alloy layer, and examples of the alloy layer include layers formed from alloys of two or more metals selected from the above group (e.g., nickel-chromium alloy, copper-nickel alloy and copper-titanium alloy). Among these, from the viewpoints of versatility in forming the conductor layer, cost, ease of patterning, and the like, a single metal layer of chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver, or copper, or an alloy layer of a nickel-chromium alloy, a copper-nickel alloy, or a copper-titanium alloy is preferred, a single metal layer of chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver, or copper, or an alloy layer of a nickel-chromium alloy is more preferred, and a single metal layer of copper is even more preferred.

[0325] The conductor layer may be a single-layer structure or a multi-layer structure in which two or more single metal layers or alloy layers made of different kinds of metals or alloys are laminated. When the conductor layer has a multi-layer structure, the layer in contact with the insulating layer is preferably a single metal layer of chromium, zinc or titanium, or an alloy layer of a nickel-chromium alloy.

[0326] The thickness of the conductor layer depends on the desired design of the printed wiring board, but is generally 3 μm to 35 μm, and preferably 5 μm to 30 μm.

[0327] In one embodiment, the conductor layer may be formed by plating. From the viewpoint of facilitating the formation of fine wiring, it is preferable to form the conductor layer by a semi-additive method. An example of forming the conductor layer by the semi-additive method will be described below.

[0328] First, a plating seed layer is formed on the surface of an insulating layer by electroless plating. Next, a mask pattern is formed on the formed plating seed layer to expose a part of the plating seed layer corresponding to a desired wiring pattern. After a metal layer is formed on the exposed plating seed layer by electrolytic plating, the mask pattern is removed. Thereafter, unnecessary plating seed layer is removed by etching or the like to form a conductor layer having a desired wiring pattern.

[0329] In another embodiment, the conductor layer may be formed using a metal foil. When the conductor layer is formed using a metal foil, it is preferable to carry out the step (V) between the steps (I) and (II). For example, after the step (I), the support is removed, and a metal foil is laminated on the exposed surface of the resin composition layer. The lamination of the resin composition layer and the metal foil may be carried out by a vacuum lamination method. The lamination conditions may be the same as those described for the step (I). Then, the step (II) is carried out to form an insulating layer. Thereafter, a conductor layer having a desired wiring pattern can be formed by a conventionally known technique such as a modified semi-additive method, using the metal foil on the insulating layer.

[0330] The metal foil can be produced by a known method such as an electrolytic method, a rolling method, etc. Commercially available metal foils include, for example, HLP foil and JXUT-III foil manufactured by JX Metals, and 3EC-III foil and TP-III foil manufactured by Mitsui Kinzoku Co., Ltd.

[0331] Alternatively, when a metal foil or a metal foil with a supporting substrate is used as the support for the resin sheet, the conductor layer may be formed using the metal foil, as described above.

[0332] <Rewiring substrate for semiconductor packages> In one embodiment, the circuit board of the present invention is a rewiring board (rewiring layer) of a semiconductor package. Hereinafter, a method for manufacturing a semiconductor package will be described.

[0333] The semiconductor package includes an insulating layer made of the cured product of the resin composition of the present invention as an insulating layer of a rewiring board. The semiconductor package may also include a sealing layer made of the cured product of the resin composition of the present invention.

[0334] A semiconductor package can be manufactured, for example, by a method including the following steps (1) to (6) using the resin composition and resin sheet of the present invention. The resin composition and resin sheet of the present invention may be used to form a rewiring formation layer (insulating layer for forming a rewiring board) in step (5) or a sealing layer in step (3). An example of forming a rewiring formation layer or a sealing layer using a resin composition or a resin sheet is shown below, but the technology for forming a rewiring formation layer or a sealing layer of a semiconductor package is publicly known, and a person skilled in the art can manufacture a semiconductor package using the resin composition and resin sheet of the present invention according to a publicly known technology. (1) A step of laminating a temporary fixing film onto a substrate; (2) a step of temporarily fixing a semiconductor chip on a temporary fixing film; (3) forming an encapsulation layer on the semiconductor chip; (4) peeling the substrate and the temporary fixing film from the semiconductor chip; (5) forming a rewiring formation layer as an insulating layer on the surface of the semiconductor chip from which the base material and the temporary fixing film have been peeled off; and (6) A process of forming a rewiring layer as a conductor layer on the rewiring formation layer.

[0335] -Process (1)- The material used for the substrate is not particularly limited. Examples of the substrate include semiconductor wafers such as silicon wafers, glass wafers, glass substrates, metal substrates such as copper, titanium, stainless steel, and cold-rolled steel (SPCC), substrates in which glass fibers are impregnated with epoxy resin or the like and subjected to a heat curing treatment (e.g., FR-4 substrates), and substrates made of bismaleimide triazine resin (BT resin).

[0336] The material of the temporary fixing film is not particularly limited as long as it can be peeled off from the semiconductor chip in step (4) and can temporarily fix the semiconductor chip. A commercially available product can be used as the temporary fixing film. An example of the commercially available product is Riva Alpha manufactured by Nitto Denko Corporation.

[0337] -Process (2)- The semiconductor chips can be temporarily fixed using known devices such as a flip chip bonder, a die bonder, etc. The layout and number of semiconductor chips can be appropriately set depending on the shape and size of the temporary fixing film, the number of semiconductor packages to be produced, etc., and for example, the semiconductor chips can be temporarily fixed by arranging them in a matrix shape of multiple rows and multiple columns.

[0338] -Process (3)- A resin composition layer of the resin sheet of the present invention is laminated on a semiconductor chip, or the resin composition of the present invention is applied onto a semiconductor chip and cured (for example, thermally cured) to form an encapsulating layer.

[0339] For example, the semiconductor chip and the resin sheet can be laminated by removing the protective film of the resin sheet and then heat-pressing the resin sheet to the semiconductor chip from the support side. Examples of the member for heat-pressing the resin sheet to the semiconductor chip (hereinafter also referred to as the "heat-pressing member") include a heated metal plate (such as a SUS plate) or a metal roll (SUS roll). It is preferable to press the heat-pressing member not directly onto the resin sheet but via an elastic material such as heat-resistant rubber so that the resin sheet can sufficiently follow the surface irregularities of the semiconductor chip. The semiconductor chip and the resin sheet may be laminated by a vacuum lamination method, and the lamination conditions are the same as those described in relation to the manufacturing method of the printed wiring board, and the preferred ranges are also the same.

[0340] After lamination, the resin composition is thermally cured to form the sealing layer under the same conditions as those described in relation to the method for producing a printed wiring board.

[0341] The support of the resin sheet may be peeled off after the resin sheet is laminated on the semiconductor chip and thermally cured, or the support may be peeled off before the resin sheet is laminated on the semiconductor chip.

[0342] When the resin composition of the present invention is applied to form a sealing layer, the application conditions are the same as the application conditions when forming the resin composition layer described in relation to the resin sheet of the present invention, and the preferred ranges are also the same.

[0343] -Process (4)- The method for peeling off the substrate and the temporary fixing film can be appropriately changed depending on the material of the temporary fixing film, and examples of the method include a method in which the temporary fixing film is heated and foamed (or expanded) to peel it off, and a method in which ultraviolet light is irradiated from the substrate side to reduce the adhesive strength of the temporary fixing film and then peeled off.

[0344] In the method of heating and foaming (or expanding) the temporary fixing film to peel it off, the heating conditions are usually 100 to 250° C. for 1 to 90 seconds or 5 to 15 minutes. In the method of irradiating ultraviolet light from the substrate side to reduce the adhesive strength of the temporary fixing film to peel it off, the irradiation dose of ultraviolet light is usually 10 mJ / cm. 2 ~1000mJ / cm 2 It is.

[0345] -Process (5)- The resin composition and resin sheet of the present invention are used to form a rewiring formation layer (insulating layer of a rewiring board).

[0346] After forming the redistribution layer, a via hole may be formed in the redistribution layer to connect the semiconductor chip to a conductor layer described later. The via hole may be formed by a known method depending on the material of the redistribution layer.

[0347] -Process (6)- The formation of the conductor layer on the rewiring formation layer may be carried out in the same manner as in step (V) described in relation to the method for producing a printed wiring board. Note that steps (5) and (6) may be repeated to alternately stack (build up) the conductor layer (rewiring layer) and the rewiring formation layer (insulating layer).

[0348] In manufacturing the semiconductor package, the steps of (7) forming a solder resist layer on the conductor layer (rewiring layer), (8) forming bumps, and (9) dicing a plurality of semiconductor packages into individual semiconductor packages may be further carried out. These steps may be carried out according to various methods used in manufacturing semiconductor packages and known to those skilled in the art.

[0349] By forming a rewiring formation layer (insulating layer) using the resin composition and resin sheet of the present invention, which can provide a cured product having excellent resin flatness and good dielectric properties and peel strength, a semiconductor package with extremely low transmission loss can be realized regardless of whether the semiconductor package is a fan-in type package or a fan-out type package. In one embodiment, the semiconductor package of the present invention is a fan-out type package. The resin composition and resin sheet of the present invention can be applied to any package, regardless of whether it is a fan-out type panel level package (FOPLP) or a fan-out type wafer level package (FOWLP). In one embodiment, the semiconductor package of the present invention is a fan-out type panel level package (FOPLP) or a fan-out type wafer level package (FOWLP).

[0350] [Semiconductor Devices] The semiconductor device of the present invention includes a layer made of a cured product of the resin composition layer of the present invention. The semiconductor device of the present invention can be produced by using the circuit board of the present invention.

[0351] Examples of the semiconductor device include various semiconductor devices used in electric appliances (for example, computers, mobile phones, digital cameras, and televisions) and vehicles (for example, motorcycles, automobiles, trains, ships, and aircraft). EXAMPLES

[0352] The present invention will be specifically described below with reference to examples. The present invention is not limited to these examples. In the following, "parts" and "%" representing amounts mean "parts by mass" and "% by mass", respectively, unless otherwise specified.

[0353] <Synthesis Example 1> Synthesis of Maleimide Resin A A maleimide resin A represented by the following formula [Mw / Mn = 1.81, m = 1.47 (mainly 1, 2 or 3)] (non-volatile components 62% by mass) was obtained by the method described in Synthesis Example 1 of the Japan Institute of Invention and Innovation Disclosure Technical Journal Publication No. 2020-500211.

[0354] [ka]

[0355] <Synthesis Example 2> Synthesis of Maleimide Resin B (I) Synthesis of intermediate amine compounds In a flask equipped with a thermometer, a condenser, a Dean-Stark trap and a stirrer, 242.4g (2.0mol) of 2-ethylaniline, 242g of xylene and 80g of activated clay were charged, and the temperature was raised to 130°C while stirring, and the temperature was held for 30 minutes. Then, 272.0g of DVB-810 (mixture of divinylbenzene / ethylstyrene (divinylbenzene / ethylstyrene = 81 / 19 (mol)%), manufactured by Nippon Steel Chemical & Material) was dropped over 2 hours, and the mixture was reacted for 1 hour. Then, the temperature was raised to 190°C over 6 hours, and the mixture was held for 10 hours. After the reaction, the mixture was air-cooled to 100°C, diluted with 300g of toluene, filtered to remove the activated clay, and low molecular weight substances such as the solvent and unreacted substances were distilled off under reduced pressure to obtain an intermediate amine compound. The amine equivalent of the intermediate amine compound was 214g / equivalent.

[0356] (II) Maleimidation A 2L flask equipped with a thermometer, a condenser, a Dean-Stark trap and a stirrer was charged with 117.7g (1.2mol) of maleic anhydride and 700g of toluene, and stirred at room temperature. Next, a mixed solution of 214g (1 equivalent) of the intermediate amine compound and 175g of DMF was dropped over 1 hour, and then reacted for 2 hours. 37.1g of p-toluenesulfonic acid monohydrate was added to the reaction solution, heated to 115°C, and the water and toluene that were azeotroped under reflux were cooled and separated, and only the toluene was returned to the system and a dehydration reaction was carried out for 5 hours. After air-cooling to room temperature, it was neutralized with 49% NaOH. Then, toluene and water were distilled off under reduced pressure at 60°C, and 600g of MEK (methyl ethyl ketone) was added to the DMF solution remaining in the flask. The solution was heated to 60°C, and the solution was separated three times with 200g of ion-exchanged water to remove salts in the solution. Sodium sulfate was further added to dry the mixture, and the mixture was concentrated under reduced pressure. The resulting reaction product was dried in vacuum at 80° C. to obtain maleimide resin B.

[0357] <Synthesis Example 3: Synthesis of vinyl resin C> 201 parts by mass of ortho-allylphenol and 1000 parts by mass of toluene were charged into a reaction vessel, and dissolved while the inside of the vessel was purged with nitrogen under reduced pressure. Then, 152 parts by mass of isophthalic acid chloride was charged and dissolved. While purging the inside of the vessel with nitrogen, 309 g of 20% aqueous sodium hydroxide solution was dropped over 3 hours. At that time, the temperature inside the system was controlled to 60°C or less. Then, the mixture was stirred for 1 hour to react. After the reaction was completed, the reaction mixture was separated and the aqueous layer was removed. This operation was repeated until the pH of the aqueous layer became 7, and toluene and the like were distilled off under heating and reduced pressure conditions to obtain vinyl resin C. The unsaturated bond equivalent of the obtained vinyl resin C was calculated to be 199 g / eq. from the charge ratio.

[0358] <Synthesis Example 4: Synthesis of vinyl resin D> In a flask equipped with a thermometer, a dropping funnel, a cooling tube, a fractionating tube, and a stirrer, 165 g of a polyaddition reaction resin of dicyclopentadiene and phenol (hydroxyl equivalent: 165 g / equivalent (eq), softening point 85 ° C.), 134 g (1.0 mol) of ortho-allylphenol, and 1200 g of toluene were charged, and the system was purged with nitrogen under reduced pressure. Then, 203 g (1.0 mol) of isophthalic acid chloride was charged, and the system was purged with nitrogen under reduced pressure. 0.6 g of tetrabutylammonium bromide was added, and while performing a nitrogen gas purging treatment, the system was controlled to 60 ° C. or less, and 412 g of a 20% aqueous sodium hydroxide solution was dropped over 3 hours, and after the dropwise addition, it was stirred for 1.0 hour. After the reaction was completed, the aqueous layer was removed by standing and separating. Water was further added to the obtained toluene layer and stirred for 15 minutes, and the aqueous layer was removed by standing and separating. This operation was repeated until the pH of the aqueous layer became 7. The non-volatile content was adjusted to 70 mass % by heat drying, thereby obtaining vinyl resin D represented by the following chemical formula.

[0359] [ka]

[0360] In the above chemical formula, each s is independently an integer of 0 or 1 or more, and the average value of r calculated from the charge ratio is 1. The dashed line in the chemical formula represents a structure obtained by reacting isophthalic acid chloride with a polyaddition reaction resin of phenol and / or ortho-allylphenol. The unsaturated bond equivalent of the obtained vinyl resin D was 428 g / eq. calculated from the charge ratio.

[0361] <Synthesis Example 5: Synthesis of Polyimide Resin E> In 400g of N,N-dimethylacetamide (DMAc) as a solvent, 46.5g of 2,2-bis[4-(3,4-dicarboxyphenoxy)phenyl]propane dianhydride (BPADA), 37.8g of 4,4'-[1,4-phenylenebis[(1-methylethylidene)-4,1-phenyleneoxy]]bisbenzenamine (BPPAN), 12.8g of dimer diamine ("PRIAMINA1075" manufactured by Croda Japan), 1.9g of 5-norbornene-2,3-dicarboxylic anhydride, and 40g of toluene as a solvent were mixed to obtain a monomer composition, which was stirred and reacted at room temperature and atmospheric pressure for 3 hours. As a result, a solution of polyamic acid was obtained.

[0362] Next, the polyamic acid solution was heated and then, while maintaining the temperature at about 160°C, the condensed water was removed azeotropically with toluene under a nitrogen stream. It was confirmed that a predetermined amount of water had accumulated in the water content receiver and that no water was flowing out. After confirmation, the reaction solution was further heated and stirred at 200°C for 1 hour. Then, it was cooled. As a result, a varnish containing a terminal olefin-modified polyimide resin E was obtained (non-volatile content 20% by mass).

[0363] [Examples 1 to 18, Comparative Examples 1 to 3] (1) Preparation of resin composition Each component was weighed out in the number of parts by mass shown in the table, and then mixed with 15 parts of MEK and 15 parts of cyclohexanone, and uniformly dispersed using a high-speed rotating mixer to obtain a resin composition (resin varnish).

[0364] <Preparation of resin sheet> As a support, a polyethylene terephthalate film ("Lumirror R80" manufactured by Toray Industries, Inc., thickness 38 μm, softening point 130° C.) that had been subjected to a release treatment with an alkyd resin-based release agent ("AL-5" manufactured by Lintec Corporation) was prepared. Each of the resin compositions obtained in Examples 1 to 18 and Comparative Examples 1 to 3 was uniformly applied onto the support using a die coater so that the thickness of the resin composition layer after drying would be 40 μm, and the coating was dried at 70° C. to 90° C. for 3 minutes to form a resin composition layer on the support. Next, a rough surface of a polypropylene film (Oji F-Tex Co., Ltd. "Alphan MA-411", thickness 15 μm) was attached as a protective film to the surface of the resin composition layer not bonded to the support, thereby obtaining a resin sheet having the support, the resin composition layer, and the protective film in this order.

[0365] <Test Example 1: Evaluation of flexibility of uncured film> The resin sheets produced in the Examples and Comparative Examples were peeled off from the protective film, and folded at an angle of 180 degrees with the support on the inside and the resin composition layer on the outside to check their flexibility. Those in which the resin composition layer was not cracked were rated as ◯, and those in which it was cracked were rated as △.

[0366] <Test Example 2: Measurement of dielectric properties (dielectric constant, dielectric tangent)> The protective film was peeled off from the resin sheets prepared in the Examples and Comparative Examples, and the resin composition layer was thermally cured by heating at 190° C. for 90 minutes, and then the support was peeled off. The obtained cured product was cut into a piece having a width of 2 mm and a length of 80 mm to prepare a test piece for evaluation. The dielectric constant and dielectric loss tangent of each test piece were measured by the cavity resonance perturbation method using an "HP8362B" manufactured by Agilent Technologies, Inc., at a measurement frequency of 5.8 GHz and a measurement temperature of 23° C. Measurements were performed on three test pieces, and the average values ​​were calculated. <Test Example 3: Measurement of Tg> The cured product was cut into test pieces with a width of about 5 mm and a length of about 15 mm, and a thermomechanical analysis was performed by the tensile load method using a thermomechanical analyzer (Rigaku's "Thermo Plus TMA8310"). After mounting the test pieces on the device, the thermal expansion coefficient (ppm) was measured twice consecutively under the measurement conditions of a load of 1 g and a heating rate of 5°C / min. In the second measurement, the glass transition temperature (Tg; °C) was calculated.

[0367] <Test Example 4: Measurement of resin flatness> (1) Preparation of inner layer board: An inner layer board (glass cloth-based epoxy resin double-sided copper-clad laminate, copper foil thickness 18 μm, board thickness 0.8 mm, Matsushita Electric Works "R1515A") was prepared, which had a copper foil surface formed with the pattern of IPC MULTI-PURPOSE TEST BOARD NO. IPC B-25 (a comb-tooth pattern with lines / spaces of 175 / 175 μm (residual copper ratio 50%)). Both sides of this inner layer board were etched with an etching agent (Mech Co., Ltd. "CZ8101") to roughen the copper foil surface.

[0368] (2) Lamination of resin sheet The protective film was peeled off from the resin sheet prepared in the examples and comparative examples to expose the resin composition layer. Using a batch-type vacuum pressure laminator (Nikko Materials Co., Ltd., 2-stage build-up laminator "CVP700"), the resin composition layer was laminated on both sides of the inner layer substrate so that it was in contact with the inner layer substrate. The lamination was performed by reducing the pressure for 30 seconds to adjust the air pressure to 13 hPa or less, and then pressing at 140°C and a pressure of 0.98 MPa for 30 seconds. Next, a heat press was performed at 110°C and a pressure of 0.54 MPa for 60 seconds.

[0369] (3) Thermal curing of the resin composition layer The inner layer substrate laminated with the resin sheet was then placed in a 130°C oven and heated for 30 minutes, and then transferred to a 180°C oven and heated for 30 minutes to thermally cure the resin composition layer and form an insulating layer.

[0370] (4) Flatness measurement The evaluation substrate was observed using a white light interference microscope (CONTOUR GT-X manufactured by Bruker) to measure the flatness of the substrate. The flatness represents the result of evaluating the difference between the maximum height and the minimum height of the surface of the insulating layer, and was evaluated according to the following criteria. ○: Less than 2μm ×: 2μm or more

[0371] <Test Example 5: Measurement of copper foil peel strength> (1) Copper foil preparation The shiny side of Mitsui Mining & Smelting Co., Ltd.'s "3EC-III" (electrolytic copper foil, 35 μm) was etched by 1 μm with a micro-etching agent (Mec Co., Ltd.'s "CZ8101") to roughen the copper surface, and then an anti-rust treatment (CL8300) was applied. Furthermore, it was heated in an oven at 130°C for 30 minutes. This copper foil is called CZ copper foil.

[0372] (2) Preparation of inner layer board Both sides of a glass cloth-based epoxy resin double-sided copper-clad laminate (copper foil thickness 18 μm, substrate thickness 0.4 mm, Panasonic "R1515A") with an inner layer circuit formed were etched 1 μm with a microetching agent (Mec "CZ8101") to roughen the copper surface.

[0373] (3) Laminating copper foil and forming an insulating layer The protective film was peeled off from the resin sheet prepared in the examples and comparative examples to expose the resin composition layer. Using a batch-type vacuum pressure laminator (Nikko Materials Co., Ltd., 2-stage build-up laminator "CVP700"), the resin composition layer was laminated on both sides of the inner layer substrate so that it was in contact with the inner layer substrate. The lamination was performed by reducing the pressure for 30 seconds to adjust the air pressure to 13 hPa or less, and then pressing at 120°C and a pressure of 0.74 MPa for 30 seconds. Next, a heat press was performed at 100°C and a pressure of 0.5 MPa for 60 seconds. The treated surface of the CZ copper foil was laminated on the resin composition layer under the same conditions as above. Then, the resin composition layer was cured under a curing condition of 200°C and 90 minutes to form an insulating layer, thereby preparing an evaluation substrate.

[0374] <Measurement of copper foil peel strength (copper foil adhesion)> The evaluation board thus prepared was cut into small pieces measuring 150 x 30 mm. A cutter was used to make a 10 mm wide, 100 mm long cut in the copper foil portion of the small piece, and one end of the copper foil was peeled off and gripped with a gripper. The load (kgf / cm) was measured when 35 mm was peeled off vertically at a speed of 50 mm / min at room temperature, and the peel strength was calculated. A tensile tester (TSE's "AC-50C-SL") was used for the measurement. The measurement was performed in accordance with the Japanese Industrial Standard (JIS C6481).

[0375] The results of Examples 1 to 18 and Comparative Examples 1 to 4 are shown in Tables 1 and 2.

[0376] [Table 1]

[0377] [Table 2]

[0378] The details of each component listed in Table 1 are as follows. <Radical polymerizable resin> MIR-3000-70MT: Aromatic maleimide resin (manufactured by Nippon Kayaku Co., Ltd., MEK / toluene mixed solution with 70% non-volatile content) MIR-5000-60T: Aromatic maleimide resin (manufactured by Nippon Kayaku Co., Ltd., toluene mixed solution with 60% non-volatile content) BMI689: Aliphatic maleimide resin (Designer Molecules, N-alkyl bismaleimide with a skeleton derived from dimer diamine) BMI1500: Aliphatic maleimide resin (Designer Molecules, N-alkyl bismaleimide with a skeleton derived from dimer diamine) OPE-2St: Vinylbenzyl-modified polyphenylene ether (Mitsubishi Gas Chemical Co., Ltd., toluene solution with 65% non-volatile content) SA9000: Methacrylic modified polyphenylene ether (SABIC Innovative Plastics) DAD: Diallyl diphenate (manufactured by Nisshoku Techno Fine Chemical Co., Ltd.) A-DOG: Dioxane glycol diacrylate (manufactured by Shin-Nakamura Chemical Co., Ltd.) DCP: Tricyclodecane dimethanol dimethacrylate (manufactured by Shin-Nakamura Chemical Co., Ltd.) ALP-d: bis[3-allyl-4-(3,4-dihydro-2H-1,3-benzoxazin-3-yl)phenyl]methane (manufactured by Shikoku Chemical Industry Co., Ltd.) Petrotac 70: Aliphatic / aromatic copolymer hydrocarbon resin with a C5 ratio of 50% (Tosoh Corporation, propenyl resin with an active group equivalent of less than 250 g / eq.) Petrotac 90: Aromatic copolymer hydrocarbon resin with a C5 ratio of 30% (Tosoh Corporation, propenyl resin with an active group equivalent of 250 g / eq. or more) FM-400: Neopentyl glycol hydroxypivalate diacrylate (a radical polymerizable resin that does not contain a ring structure in the main skeleton and has an active group equivalent of less than 250 g / eq., manufactured by Nippon Kayaku Co., Ltd.) <Inorganic filler> SO-C2: Spherical silica (manufactured by Admatechs, average particle size 0.5 μm, specific surface area 5.8 m 2 / g), surface-treated with a silane coupling agent ("KBM-573" manufactured by Shin-Etsu Chemical Co., Ltd.) UFP-30: Spherical silica (manufactured by Denka, average particle size 0.3 μm, specific surface area 30 m 2 / g), surface-treated with a silane coupling agent ("KBM-573" manufactured by Shin-Etsu Chemical Co., Ltd.) Hypresica FH: Hollow silica (Ube Exsymo, average particle size 0.5 μm, porosity 30-50%), surface-treated with a silane coupling agent (Shin-Etsu Chemical "KBM-573") <Thermoplastic resin> FPC2136: Polycarbonate resin (manufactured by Mitsubishi Gas Chemical Co., Ltd.) YX7553BH30: Phenoxy resin (manufactured by Mitsubishi Chemical Corporation, a 1:1 solution of MEK with 30% non-volatile content and cyclohexanone) <Thermosetting resin> NC-3000L: Biphenyl type epoxy resin (manufactured by Nippon Kayaku Co., Ltd., epoxy equivalent: approx. 269g / eq.) <Hardening agent> LA3018-50P: Triazine skeleton-containing phenolic curing agent (DIC Corporation, active group equivalent weight approx. 151g / eq., non-volatile content 50% in 2-methoxypropanol solution) V-03: Carbodiimide-based curing agent (Nisshinbo Chemical Co., Ltd., active group equivalent weight approx. 216 g / eq., non-volatile content 50% in toluene solution) HPC8000-65T: Active ester compound (DIC, active ester equivalent weight approx. 223g / eq., non-volatile content 65% in toluene solution) <Radical polymerization initiator> Luperox DTA: Di-t-amyl peroxide (Arkema Yoshitomi Co., Ltd.) Perbutyl C: t-butylcumyl peroxide (NOF Corporation) Perbutyl P: bis(1-tert-butylperoxy-1-methylethyl)benzene (NOF Corporation) Perhexyl D: Di-t-hexyl peroxide (NOF Corporation) <Curing accelerator> 1B2PZ: Imidazole-based curing accelerator (manufactured by Shikoku Chemical Industry Co., Ltd.)

Claims

1. A radical polymerizable resin A containing a ring structure in its main skeleton, and A resin composition containing di-t-amyl peroxide.

2. The resin composition according to claim 1 , wherein the radical polymerizable resin A comprises two or more kinds of radical polymerizable resins.

3. The resin composition according to claim 2, wherein the radical polymerizable resin A contains at least a resin selected from the group consisting of a maleimide resin, a terminal double bond-modified polyphenylene ether resin, and a (meth)acrylic resin.

4. The resin composition according to claim 1 , wherein the radical polymerizable resin A comprises a radical polymerizable resin having a molecular weight of 1,000 or less.

5. The resin composition according to claim 1, wherein the radical polymerizable resin A comprises a radical polymerizable resin (A-1) having an active group equivalent of 250 g / eq. or more and a radical polymerizable resin (A-2) having an active group equivalent of less than 250 g / eq.

6. The resin composition according to claim 5, wherein the content of the radical polymerizable resin (A-2) is less than the content of the radical polymerizable resin (A-1).

7. The resin composition according to claim 5, wherein the content of the radical polymerizable resin (A-2) is 50% or less of the content of the radical polymerizable resin (A-1).

8. The resin composition according to claim 1 , wherein the content of the radical polymerizable resin A is 40% by mass or more when the resin component in the resin composition is 100% by mass.

9. 2. The resin composition according to claim 1, wherein the content of di-t-amyl peroxide is 0.1% by mass or more and 2.5% by mass or less, when the resin component in the resin composition is 100% by mass.

10. The resin composition according to claim 1 , further comprising an inorganic filler.

11. The resin composition according to claim 10, wherein the content of the inorganic filler is 30% by mass or more when the nonvolatile components in the resin composition are taken as 100% by mass.

12. The resin composition according to claim 1 , further comprising a thermoplastic resin.

13. The resin composition according to claim 12, wherein the content of the thermoplastic resin is 0.1% by mass or more and 5.0% by mass or less, when the resin component in the resin composition is 100% by mass.

14. The resin composition according to claim 1, which is used for an insulating layer of a circuit board.

15. A resin sheet comprising a support and a layer of the resin composition according to any one of claims 1 to 14 provided on the support.

16. The resin sheet according to claim 15, wherein the support is a thermoplastic resin film or a metal foil.

17. A cured product of the resin composition according to any one of claims 1 to 14.

18. A circuit board comprising an insulating layer made of a cured product of the resin composition according to any one of claims 1 to 14.

19. A semiconductor device comprising the circuit board according to claim 18.

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