JP7793889B2 - resin composition - Google Patents

Description

The present invention relates to a resin composition containing a polycarbonate resin. It also relates to a cured product, a sheet-like laminate material, a resin sheet, a printed wiring board, and a semiconductor device obtained using the resin composition.

A known manufacturing technique for printed wiring boards is the build-up method, in which insulating layers and conductor layers are alternately stacked. In build-up manufacturing methods, insulating layers are generally formed by curing a resin composition. In recent years, there has been a demand for insulating layers with a lower dielectric constant (Dk).

Incidentally, polycarbonate resins with alicyclic structures have been known to date (Patent Document 1).

Japanese Patent Application Laid-Open No. 2018-197282

The objective of the present invention is to provide a resin composition that can produce a cured product with a lower dielectric constant (Dk).

In order to achieve the objectives of the present invention, the inventors conducted extensive research and discovered, unexpectedly, that by using a resin composition containing (A) a polycarbonate resin and (B) an epoxy resin, where component (A) contains a polycarbonate resin having a repeating structural unit represented by formula (A1) described below, it is possible to obtain a cured product with a lower relative dielectric constant (Dk), which led to the completion of the present invention.

That is, the present invention includes the following.
[1] A resin composition comprising (A) a polycarbonate resin and (B) an epoxy resin,
The component (A) is represented by the formula (A1):

[In the formula,
Ring A and ring B each independently represent an aromatic ring which may have a substituent;
Ring X represents a non-aromatic carbocyclic ring having 7 or more carbon atoms which may have a substituent.
A resin composition comprising a polycarbonate resin having a repeating structural unit represented by the formula:
[2] The component (A) is represented by the formula (A3):

[In the formula,
R ¹ and R ² each independently represent a hydrogen atom, an alkyl group, or an aryl group;
^R3 and ^R4 each independently represent an alkyl group or an aryl group;
a and b each independently represent 0, 1, 2, 3, or 4;
n represents an integer of 6 or more.
The resin composition according to the above [1], comprising a polycarbonate resin having a repeating structural unit represented by the following formula:
[3] The resin composition according to the above [1] or [2], wherein the weight average molecular weight (Mw) of the component (A) is 10,000 or less.
[4] The resin composition according to any one of the above [1] to [3], wherein the hydroxyl group content of the component (A) is 0.05 mmol/g or less.
[5] The resin composition according to any one of [1] to [4] above, wherein the content of the component (A) is 10% by mass or more, when the total amount of non-volatile components in the resin composition is 100% by mass.
[6] The resin composition according to any one of [1] to [5] above, wherein the content of the component (A) is 50% by mass or less, when the total amount of non-volatile components in the resin composition is 100% by mass.
[7] The resin composition according to any one of [1] to [6] above, wherein the content of the component (B) is 20% by mass or less, when the total amount of non-volatile components in the resin composition is 100% by mass.
[8] The resin composition according to any one of the above [1] to [7], further comprising (C) an inorganic filler.
[9] The resin composition according to the above [8], wherein the component (C) is silica.
[10] The resin composition according to the above [8] or [9], wherein the content of the component (C) is 40% by mass or more, when the total amount of non-volatile components in the resin composition is 100% by mass.
[11] The resin composition according to any one of the above [1] to [10], further comprising (D) an epoxy resin curing agent.
[12] The resin composition according to the above [11], wherein the component (D) contains an active ester curing agent.
[13] The resin composition according to any one of the above [1] to [12], further comprising (E) a radically polymerizable compound.
[14] The resin composition according to any one of [1] to [13] above, wherein the dielectric loss tangent (Df) of the cured product of the resin composition is 0.0040 or less when measured at 5.8 GHz and 23 ° C.
[15] The resin composition according to any one of [1] to [14], wherein the dielectric constant (Dk) of the cured product of the resin composition is 3.1 or less when measured at 5.8 GHz and 23°C.
[16] A cured product of the resin composition according to any one of [1] to [15] above.
[17] A sheet-like laminate material containing the resin composition according to any one of [1] to [15] above.
[18] A resin sheet comprising a support and a resin composition layer formed from the resin composition according to any one of [1] to [15] above, provided on the support.
[19] A printed wiring board having an insulating layer made of a cured product of the resin composition according to any one of [1] to [15] above.
[20] A semiconductor device comprising the printed wiring board according to [19] above.

The resin composition of the present invention makes it possible to obtain a cured product with a lower dielectric constant (Dk).

The present invention will now be described in detail 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.

<Resin composition>
The resin composition of the present invention comprises (A) a polycarbonate resin and (B) an epoxy resin, and the component (A) is a compound represented by formula (A1):

[In the formula,
Ring A and ring B each independently represent an aromatic ring which may have a substituent;
Ring X represents a non-aromatic carbocyclic ring having 7 or more carbon atoms which may have a substituent.
The resin composition contains a polycarbonate resin having a repeating structural unit represented by the following formula: By using such a resin composition, it is possible to obtain a cured product having a lower relative dielectric constant (Dk).

The resin composition of the present invention may contain optional components in addition to (A) polycarbonate resin and (B) epoxy resin. Examples of optional components include (C) inorganic filler, (D) epoxy resin curing agent, (E) radical polymerizable compound, (F) curing accelerator, (G) radical polymerization initiator, (H) other additives, and (I) organic solvent. Each component contained in the resin composition is described in detail below.

<(A) Polycarbonate Resin>
The resin composition of the present invention contains (A) a polycarbonate resin. (A) The polycarbonate resin is a resin containing a repeating unit having a carbonate ester, and can be obtained, for example, by polycondensation of a diol component and a carbonate diester component.

(A) Polycarbonate resin has the formula (A1):

[In the formula,
Ring A and ring B each independently represent an aromatic ring which may have a substituent;
Ring X represents a non-aromatic carbocyclic ring having 7 or more carbon atoms which may have a substituent.
The polycarbonate resin includes a polycarbonate resin having a repeating structural unit represented by the formula (A1). The repeating structural unit represented by the formula (A1) may be of one type or of two or more types in one molecule.

Ring A and ring B each independently represent an aromatic ring which may have a substituent.

An aromatic ring refers to a ring that conforms to Hückel's rule, in which the number of electrons contained in the π-electron system on the ring is 4p+2 (p is a natural number). An aromatic ring may be an aromatic carbocyclic ring containing only carbon atoms as ring constituent atoms, or an aromatic heterocyclic ring containing heteroatoms such as oxygen, nitrogen, or sulfur atoms in addition to carbon atoms as ring constituent atoms. In one embodiment, an aromatic carbocyclic ring is preferred. In one embodiment, the aromatic ring is preferably a 5- to 14-membered aromatic ring, more preferably a 6- to 14-membered aromatic ring, and even more preferably a 6- to 10-membered aromatic ring. Specific examples of suitable aromatic rings include a benzene ring, a naphthalene ring, an anthracene ring, and a phenanthrene ring. A benzene ring or a naphthalene ring is more preferred, and a benzene ring is particularly preferred.

In this specification, the substituent is not particularly limited, but examples include monovalent substituents such as an alkyl group, an alkenyl group, an aryl group, an aryl-alkyl group (an alkyl group substituted with an aryl group), an alkyl-aryl group (an aryl group substituted with an alkyl group), an alkyl-oxy group, an alkenyl-oxy group, an aryl-oxy group, an alkyl-carbonyl group, an alkenyl-carbonyl group, an aryl-carbonyl group, an alkyl-oxy-carbonyl group, an alkenyl-oxy-carbonyl group, an aryl-oxy-carbonyl group, an alkyl-carbonyl-oxy group, an alkenyl-carbonyl-oxy group, and an aryl-carbonyl-oxy group, and, if substitutable, may also include divalent substituents such as an oxo group (=O).

The term "alkyl group" refers to a linear, branched, and/or cyclic monovalent aliphatic saturated hydrocarbon group. Unless otherwise specified, the alkyl group is preferably an alkyl group having 1 to 14 carbon atoms, more preferably an alkyl group having 1 to 10 carbon atoms, and even more preferably an alkyl group having 1 to 6 carbon atoms. Examples of the alkyl group include methyl, ethyl, propyl, isopropyl, butyl, isobutyl, sec-butyl, tert-butyl, pentyl, hexyl, heptyl, octyl, nonyl, decyl, cyclopentyl, cyclohexyl, methylcyclohexyl, dimethylcyclohexyl, trimethylcyclohexyl, cyclopentylmethyl, and cyclohexylmethyl. The term "alkenyl group" refers to a linear, branched, and/or cyclic monovalent aliphatic unsaturated hydrocarbon group having at least one carbon-carbon double bond. Unless otherwise specified, the alkenyl group is preferably an alkenyl group having 2 to 14 carbon atoms, more preferably an alkenyl group having 2 to 10 carbon atoms, and even more preferably an alkenyl group having 2 to 6 carbon atoms. Examples of alkenyl groups include vinyl, propenyl, butenyl, pentenyl, hexenyl, heptenyl, octenyl, nonenyl, decenyl, and cyclohexenyl. The aryl group refers to a monovalent aromatic hydrocarbon group formed by removing one hydrogen atom from an aromatic carbon ring. Unless otherwise specified, the aryl group is preferably an aryl group having 6 to 14 carbon atoms, and particularly preferably an aryl group having 6 to 10 carbon atoms. Examples of aryl groups include phenyl, 1-naphthyl, and 2-naphthyl.

Ring A and Ring B are preferably each independently a benzene ring optionally substituted with a group selected from an alkyl group, an alkenyl group, an aryl group, an aryl-alkyl group, an alkyl-aryl group, an alkyl-oxy group, an alkenyl-oxy group, and an aryl-oxy group; or a naphthalene ring optionally substituted with a group selected from an alkyl group, an alkenyl group, an aryl group, an aryl-alkyl group, an alkyl-aryl group, an alkyl-oxy group, an alkenyl-oxy group, and an aryl-oxy group. Ring A and Ring B are more preferably each independently a benzene ring optionally substituted with a group selected from an alkyl group, an aryl group, an aryl-alkyl group, and an alkyl-aryl group; or a naphthalene ring optionally substituted with a group selected from an alkyl group, an aryl group, an aryl-alkyl group, and an alkyl-aryl group. Ring A and Ring B are even more preferably each independently a benzene ring optionally substituted with a group selected from an alkyl group and an aryl group; or a naphthalene ring optionally substituted with a group selected from an alkyl group and an aryl group. Ring A and ring B are particularly preferably each independently an (unsubstituted) benzene ring or an (unsubstituted) naphthalene ring.

Ring X represents a non-aromatic carbocyclic ring having 7 or more carbon atoms, which may have a substituent.

A non-aromatic carbocycle is a carbocycle that does not contain an aromatic carbocycle. A non-aromatic carbocycle has only carbon atoms as ring-constituting atoms. A non-aromatic carbocycle may be a saturated carbocycle consisting of only single bonds, or a non-aromatic unsaturated carbocycle having at least one of a double bond and a triple bond, but a saturated carbocycle consisting of only single bonds is preferable. A non-aromatic carbocycle having 7 or more carbon atoms is preferably a non-aromatic carbocycle having 8 to 21 carbon atoms, more preferably a non-aromatic carbocycle having 9 to 17 carbon atoms, even more preferably a non-aromatic carbocycle having 10 to 14 carbon atoms, and even more preferably a non-aromatic carbocycle having 11 to 13 carbon atoms. Specific preferred examples of the non-aromatic carbocyclic ring having 7 or more carbon atoms include, for example, a cycloheptane ring, a cyclooctane ring, a cyclononane ring, a cyclodecane ring, a cycloundecane ring, a cyclododecane ring, a cyclotridecane ring, a cyclotetradecane ring, a cyclopentadecane ring, a cyclohexadecane ring, a cycloheptadecane ring, a cyclooctadecane ring, and a cyclononadecane ring; a bicyclo[ saturated bicyclic carbocyclic rings having 7 or more carbon atoms, such as a bicyclo[5.2.1.0 2,6 ]heptane ring (norbornane ring), a bicyclo[4.4.0]decane ring (decalin ring), a bicyclo[5.3.0]decane ring, a bicyclo[4.3.0]nonane ring (hydrindane ring), a bicyclo[3.2.1]octane ring, a bicyclo[5.4.0]undecane ring, a bicyclo[3.3.0]octane ring, and a bicyclo[ ^3.3.1 ]nonane ring; saturated tricyclic carbocyclic rings having 7 or more carbon atoms, such as a tricyclo[5.2.1.0 ^2,6 ]decane ring (tetrahydrodicyclopentadiene ring), a tricyclo[3.3.1.1 ^3,7 ]decane ring (adamantane ring), and a tricyclo[6.2.1.0 ^2,7 ]undecane ring; and saturated five-ring carbocyclic rings having 7 or more carbon atoms such as a pentacyclo[9.2.1.1 ^4,7 . ^{0 2,1 0.0 3,8} ]pentadecane ring and a pentacyclo[6.5.1.1 ^3,6 . 0 ^2,7 . 0 ^9,13 ]pentadecane ring (tetrahydrotricyclopentadiene ring), and preferably a monocyclic saturated carbocyclic ring having 7 or more carbon atoms.

Ring X is preferably a non-aromatic carbocyclic ring having 7 or more carbon atoms which may be substituted with a group selected from an alkyl group, an alkenyl group, an aryl group, an aryl-alkyl group, an alkyl-aryl group, an alkyl-oxy group, an alkenyl-oxy group, an aryl-oxy group, and an oxo group. Ring X is more preferably a non-aromatic carbocyclic ring having 7 or more carbon atoms which may be substituted with a group selected from an alkyl group, an aryl group, an aryl-alkyl group, an alkyl-aryl group, and an oxo group. Ring X is even more preferably a non-aromatic carbocyclic ring having 7 or more carbon atoms which may be substituted with a group selected from an alkyl group and an aryl group. Ring X is particularly preferably an (unsubstituted) non-aromatic carbocyclic ring having 7 or more carbon atoms.

In one embodiment, the polycarbonate resin (A) preferably has the formula (A2):

[In the formula,
R ¹ and R ² each independently represent a hydrogen atom, an alkyl group, or an aryl group;
n represents an integer of 6 or more;
Other symbols are as above.]
The polycarbonate resin includes a polycarbonate resin having a repeating structural unit represented by the formula (A2): The repeating structural unit represented by the formula (A2) may be of one type or of two or more types in one molecule.

^R1 and ^R2 each independently represent a hydrogen atom, an alkyl group, or an aryl group. ^R1 and ^R2 each independently represent a hydrogen atom or an alkyl group, and more preferably a hydrogen atom.

n represents an integer of 6 or greater. n is preferably 7 or greater, more preferably 8 or greater, even more preferably 9 or greater, and even more preferably 10 or greater. The upper limit of n is preferably 20 or less, more preferably 16 or less, even more preferably 13 or less, and even more preferably 12 or less. n is particularly preferably 11.

In one embodiment, the (A) polycarbonate resin is more preferably represented by formula (A3):

[In the formula,
^R3 and ^R4 each independently represent an alkyl group or an aryl group;
a and b each independently represent 0, 1, 2, 3, or 4;
Other symbols are as above.]
The polycarbonate resin includes a polycarbonate resin having a repeating structural unit represented by the formula (A3). The repeating structural unit represented by the formula (A3) may be of one type or of two or more types in one molecule.

^R3 and ^R4 each independently represent an alkyl group or an aryl group, ^and are preferably ^each independently an alkyl group.

a and b each independently represent 0, 1, 2, 3, or 4. a and b each independently represent preferably 0, 1, 2, or 3, more preferably 0, 1, or 2, even more preferably 0 or 1, and particularly preferably 0.

In one embodiment, the polycarbonate resin (A) is more preferably represented by formula (A4):

[In the formula, each symbol is as defined above.]
The polycarbonate resin includes a polycarbonate resin having a repeating structural unit represented by the formula (A4). The repeating structural unit represented by the formula (A4) may be of one type or of two or more types in one molecule.

In one embodiment, the average number of repeating units (average degree of polymerization) of the repeating structural unit represented by formula (A1) (including structural units represented by formulae (A2) to (A4)) in the (A) polycarbonate resin is preferably 2 or more, more preferably 2 to 10, even more preferably 2 to 8, still more preferably 3 to 6, and particularly preferably 4 to 5.

From the viewpoint of further reducing the dielectric dissipation factor of the cured product, the (A) polycarbonate resin is preferably a polycarbonate resin in which the terminals of the resin molecules are relatively high in non-functional inactive groups such as naphthyl groups, xylyl groups, tert-butylphenyl groups, and phenyl groups, and in which the hydroxyl group content (particularly the phenolic hydroxyl group content) is low. From the viewpoint of further reducing the dielectric dissipation factor of the cured product, in one embodiment, the hydroxyl group content of the (A) polycarbonate resin is preferably 0.5 mmol/g or less, more preferably 0.1 mmol/g or less, even more preferably 0.05 mmol/g or less, and particularly preferably 0.02 mmol/g or less.

In one embodiment, the weight average molecular weight (Mw) of the (A) polycarbonate resin is preferably 50,000 or less, more preferably 20,000 or less, even more preferably 10,000 or less, and particularly preferably 5,000 or less. In one embodiment, the lower limit is preferably 1,000 or more, more preferably 2,000 or more, even more preferably 2,500 or more, and particularly preferably 3,000 or more. The weight average molecular weight (Mw) of the resin can be measured as a polystyrene-equivalent value by gel permeation chromatography (GPC).

In one embodiment, the number average molecular weight (Mn) of the (A) polycarbonate resin is preferably 30,000 or less, more preferably 10,000 or less, even more preferably 5,000 or less, and particularly preferably 3,000 or less. In one embodiment, the lower limit is preferably 1,000 or more, more preferably 1,200 or more, even more preferably 1,400 or more, and particularly preferably 1,500 or more. The number average molecular weight (Mn) of the resin can be measured as a polystyrene-equivalent value by gel permeation chromatography (GPC).

In one embodiment, the polydispersity (Mw/Mn) of the (A) polycarbonate resin is preferably in the range of 1.1 to 10.0, more preferably in the range of 1.5 to 5.0, and particularly preferably in the range of 2.0 to 3.0.

(A) Commercially available polycarbonate resins include, for example, "Ph-PCO-BPCDE," "PCO-BPCDE-R," and "PCO-BPCDE" manufactured by Honshu Chemical Industry Co., Ltd., and one or more of these may be used.

The content of (A) polycarbonate resin in the resin composition is not particularly limited, but is preferably 70% by mass or less, more preferably 50% by mass or less, even more preferably 40% by mass or less, even more preferably 30% by mass or less, and particularly preferably 20% by mass or less, based on 100% by mass of non-volatile components in the resin composition. The lower limit of the content of (A) polycarbonate resin in the resin composition is not particularly limited, but is preferably 0.1% by mass or more, more preferably 0.5% by mass or more, even more preferably 1% by mass or more, even more preferably 5% by mass or more, and particularly preferably 10% by mass or more, based on 100% by mass of non-volatile components in the resin composition.

<(B) Epoxy Resin>
The resin composition of the present invention contains (B) an epoxy resin. (B) The epoxy resin is a curable resin having an epoxy group.

(B) Examples of epoxy resins include bixylenol-type epoxy resins, bisphenol A-type epoxy resins, bisphenol F-type epoxy resins, bisphenol S-type epoxy resins, bisphenol AF-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, and glycidyl ether-type epoxy resins. Examples of (B) epoxy resins include ester-type epoxy resins, cresol novolac-type epoxy resins, phenol aralkyl-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, tetraphenylethane-type epoxy resins, isocyanurate-type epoxy resins, and phenolphthalimidine-type epoxy resins. The (B) epoxy resins may be used alone or in combination of two or more.

The resin composition preferably contains, as the (B) epoxy resin, an epoxy resin having two or more epoxy groups per molecule. The proportion of the epoxy resin having two or more epoxy groups per molecule relative to 100% by mass of the non-volatile components of the (B) epoxy resin is preferably 50% by mass or more, more preferably 60% by mass or more, and particularly preferably 70% by mass or more.

Epoxy resins include those that are liquid at a temperature of 20°C (hereinafter sometimes referred to as "liquid epoxy resins") and those that are solid at a temperature of 20°C (hereinafter sometimes referred to as "solid epoxy resins"). The resin composition of the present invention may contain only liquid epoxy resins as epoxy resins, or only solid epoxy resins, or a combination of liquid and solid epoxy resins.

Preferably, the liquid epoxy resin is one having two or more epoxy groups per molecule.

Preferred liquid epoxy resins are glycerol-type epoxy resins, bisphenol A-type epoxy resins, bisphenol F-type epoxy resins, bisphenol AF-type epoxy resins, naphthalene-type epoxy resins, glycidyl ester-type epoxy resins, glycidyl amine-type epoxy resins, phenol novolac-type epoxy resins, alicyclic epoxy resins having an ester skeleton, cyclohexanedimethanol-type epoxy resins, cycloaliphatic glycidyl ethers, and epoxy resins having a butadiene structure, with glycerol-type epoxy resins, cycloaliphatic glycidyl ethers, bisphenol A-type epoxy resins, and bisphenol F-type epoxy resins being more preferred.

Specific examples of liquid epoxy resins include Nagase ChemteX's "EX-992L," Mitsubishi Chemical's "YX7400," and DIC's "HP4032," "HP4032D," and "HP4032SS" (naphthalene-type epoxy resins); Mitsubishi Chemical's "828US," "828EL," "jER828EL," "825," and "Epikote 828EL" (bisphenol A-type epoxy resins); Mitsubishi Chemical's "jER807," "1750" ( bisphenol F type epoxy resin); Mitsubishi Chemical Corporation's "jER152" (phenol novolac type epoxy resin); Mitsubishi Chemical Corporation's "630", "630LSD", and "604" (glycidylamine type epoxy resin); ADEKA Corporation's "ED-523T" (glycilol type epoxy resin); ADEKA Corporation's "EP-3950L" and "EP-3980S" (glycidylamine type epoxy resin); ADEKA Corporation's "EP-4088S" (dicyclopentasiloxane type epoxy resin). bisphenol A type epoxy resin); "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) ), Daicel Corporation's "PB-3600," Nippon Soda Co., Ltd.'s "JP-100" and "JP-200" (epoxy resins with a butadiene structure); Nippon Steel Chemical & Material Co., Ltd.'s "ZX1658" and "ZX1658GS" (liquid 1,4-glycidylcyclohexane-type epoxy resin); Osaka Gas Chemicals Co., Ltd.'s "EG-280" (fluorene structure-containing epoxy resin); and Nagase ChemteX Corporation's "EX-201" (cyclic aliphatic glycidyl ether).

As a solid epoxy resin, a solid epoxy resin having three or more epoxy groups per molecule is preferred, and an aromatic solid epoxy resin having three or more epoxy groups per molecule is more preferred.

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.

Specific examples of solid epoxy resins include DIC Corporation's "HP4032H" (naphthalene-type epoxy resin); DIC Corporation's "HP-4700" and "HP-4710" (naphthalene-type tetrafunctional epoxy resins); DIC Corporation's "N-690" (cresol novolac-type epoxy resin); DIC Corporation's "N-695" (cresol novolac-type epoxy resin); DIC Corporation's "HP-7200," "HP-7200HH," "HP-7200H," and "HP-7200L" (dicyclopentadiene-type epoxy resins); and DIC Corporation's "EXA-7311." "EXA-7311-G3", "EXA-7311-G4", "EXA-7311-G4S", "HP6000" (naphthylene ether type epoxy resin); "EPPN-502H" (trisphenol type epoxy resin) manufactured by Nippon Kayaku Co., Ltd.; "NC7000L" (naphthol novolac type epoxy resin) manufactured by Nippon Kayaku Co., Ltd.; "NC3000H", "NC3000", "NC3000L", "NC3000FH", "NC3100" (biphenyl type epoxy resin) manufactured by Nippon Kayaku Co., Ltd.; "ESN475V", "ESN4 100V" (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", and "YL7890" (bixylenol-type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "YL6121" (biphenyl-type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "YX8800" (anthracene-type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "Y" manufactured by Mitsubishi Chemical Corporation Examples include X7700 (phenol aralkyl type epoxy resin); PG-100 and CG-500 manufactured by Osaka Gas Chemicals; YL7760 (bisphenol AF type epoxy resin) manufactured by Mitsubishi Chemical; YL7800 (fluorene type epoxy resin) manufactured by Mitsubishi Chemical; jER1010 (bisphenol A type epoxy resin) manufactured by Mitsubishi Chemical; jER1031S (tetraphenylethane type epoxy resin) manufactured by Mitsubishi Chemical; and WHR991S (phenolphthalimidine type epoxy resin) manufactured by Nippon Kayaku Co., Ltd. These may be used alone or in combination of two or more.

When a combination of liquid epoxy resin and solid epoxy resin is used as the (B) epoxy resin, the mass ratio thereof (liquid epoxy resin:solid epoxy resin) is preferably 10:1 to 1:50, more preferably 2:1 to 1:20, and particularly preferably 1:1 to 1:10.

The epoxy equivalent of (B) 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 resin per equivalent of epoxy groups. This epoxy equivalent can be measured in accordance with JIS K7236.

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

The content of (B) epoxy resin in the resin composition is not particularly limited, but is preferably 30% by mass or less, more preferably 25% by mass or less, even more preferably 20% by mass or less, even more preferably 15% by mass or less, and particularly preferably 10% by mass or less, based on 100% by mass of the non-volatile components in the resin composition. The lower limit of the content of (B) epoxy resin in the resin composition is not particularly limited, but is preferably 0.01% by mass or more, more preferably 0.1% by mass or more, even more preferably 0.5% by mass or more, even more preferably 1% by mass or more, and particularly preferably 3% by mass or more, based on 100% by mass of the non-volatile components in the resin composition.

The mass ratio of the (A) polycarbonate resin to the (B) epoxy resin in the resin composition (component (A)/component (B)) is not particularly limited, but is preferably 0.1 or greater, more preferably 0.5 or greater, even more preferably 1 or greater, and particularly preferably 2 or greater. The upper limit of the mass ratio of the (A) polycarbonate resin to the (B) epoxy resin in the resin composition (component (A)/component (B)) is not particularly limited, but is preferably 1000 or less, more preferably 100 or less, even more preferably 50 or less, and particularly preferably 10 or less.

<(C) Inorganic filler>
The resin composition of the present invention may contain an inorganic filler (C) as an optional component. The inorganic filler (C) is contained in the resin composition in the form of particles.

(C) An inorganic compound is used as the inorganic filler material. Examples of (C) inorganic filler materials include silica, alumina, glass, cordierite, silicon oxide, barium sulfate, barium carbonate, talc, clay, mica powder, zinc oxide, hydrotalcite, boehmite, aluminum hydroxide, magnesium hydroxide, calcium carbonate, magnesium carbonate, magnesium oxide, boron nitride, aluminum nitride, manganese nitride, aluminum borate, strontium carbonate, strontium titanate, calcium titanate, magnesium titanate, bismuth titanate, titanium oxide, zirconium oxide, barium titanate, barium titanate zirconate, barium zirconate, calcium zirconate, zirconium phosphate, and zirconium tungstate phosphate. Among these, silica is particularly preferred. Examples of silica include amorphous silica, fused silica, crystalline silica, synthetic silica, and hollow silica. Spherical silica is preferred. (C) The inorganic filler may be used alone or in a combination of two or more types in any ratio.

(C) Commercially available inorganic fillers include, for example, "UFP-30" manufactured by Denka Chemical Industry Co., Ltd.; "SP60-05" and "SP507-05" manufactured by Nippon Steel & Sumikin Materials Co., Ltd.; "YC100C," "YA050C," "YA050C-MJE," and "YA010C" manufactured by Admatechs Co., Ltd.; "UFP-30" manufactured by Denka Company Limited; "Silfil NSS-3N," "Silfil NSS-4N," and "Silfil NSS-5N" manufactured by Tokuyama Corporation; "SC2500SQ," "SO-C4," "SO-C2," and "SO-C1" manufactured by Admatechs Co., Ltd.; and "DAW-03" and "FB-105FD" manufactured by Denka Company Limited.

The average particle size of (C) inorganic filler is not particularly limited, but is preferably 10 μm or less, more preferably 5 μm or less, even more preferably 2 μm or less, even more preferably 1 μm or less, and particularly preferably 0.7 μm or less. The lower limit of the average particle size of (C) inorganic filler is not particularly limited, but is preferably 0.01 μm or more, more preferably 0.05 μm or more, even more preferably 0.1 μm or more, and particularly preferably 0.2 μm or more. The average particle size of (C) inorganic filler can be measured using a laser diffraction/scattering method based on Mie scattering theory. Specifically, a particle size distribution of the inorganic filler is created on a volume basis using a laser diffraction/scattering particle size distribution analyzer, and the median diameter is used as the average particle size. A measurement sample can be prepared by weighing 100 mg of inorganic filler and 10 g of methyl ethyl ketone into a vial and ultrasonically dispersing for 10 minutes. The measurement sample was measured using a laser diffraction particle size distribution analyzer, with blue and red light source wavelengths used and a flow cell system to measure the volumetric particle size distribution of the inorganic filler, and the average particle size was calculated as the median diameter from the obtained particle size distribution. Examples of laser diffraction particle size distribution analyzers include the "LA-960" manufactured by Horiba, Ltd.

The specific surface area of (C) inorganic filler is not particularly limited, but is preferably 0.1 m ² /g or more, more preferably 0.5 m ² /g or more, even more preferably 1 m ² /g or more, and particularly preferably 3 m ² /g or more. The upper limit of the specific surface area of (C) inorganic filler is not particularly limited, but is preferably 100 m ² /g or less, more preferably 70 m ² /g or less, even more preferably 50 m ² /g or less, and particularly preferably 40 m ² /g or less. The specific surface area of the inorganic filler can be obtained according to the BET method by adsorbing nitrogen gas onto the surface of a sample using a specific surface area measuring device (Macsorb HM-1210 manufactured by Mountech Co., Ltd.) and calculating the specific surface area using the BET multipoint method.

(C) From the viewpoint of improving moisture resistance and dispersibility, it is preferable that the inorganic filler be treated with a surface treatment agent. Examples of surface treatment agents include fluorine-containing silane coupling agents, aminosilane coupling agents, epoxysilane coupling agents, mercaptosilane coupling agents, silane coupling agents, alkoxysilanes, organosilazane compounds, and titanate coupling agents. Furthermore, one type of surface treatment agent may be used alone, or two or more types may be used in any combination.

Commercially available surface treatment agents include, for example, 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), Shin-Etsu Chemical Co., Ltd.'s "SZ-31" (hexamethyldisilazane), Shin-Etsu Chemical Co., Ltd.'s "KBM103" (phenyltrimethoxysilane), Shin-Etsu Chemical Co., Ltd.'s "KBM-4803" (long-chain epoxy-type silane coupling agent), and Shin-Etsu Chemical Co., Ltd.'s "KBM-7103" (3,3,3-trifluoropropyltrimethoxysilane).

From the perspective of improving the dispersibility of the inorganic filler, it is preferable that the degree of surface treatment with the surface treatment agent falls within a specified range. Specifically, 100% by mass of inorganic filler is preferably surface-treated with 0.2% to 5% by mass of surface treatment agent, more preferably 0.2% to 3% by mass, and even more preferably 0.3% to 2% by mass.

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 preferably 0.02 mg/ ^m2 or more, more preferably 0.1 mg/ ^m2 or more, and even more preferably 0.2 mg/ ^m2 or more. On the other hand, from the viewpoint of preventing an increase in the melt viscosity of the resin composition or the melt viscosity in a sheet form, the amount of carbon per unit surface area is preferably 1.0 mg/ ^m2 or less, more preferably 0.8 mg/ ^m2 or less, and even more preferably 0.5 mg/ ^m2 or less.

(C) 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 solids, the amount of carbon per unit surface area of the inorganic filler can be measured using a carbon analyzer. An example of a carbon analyzer that can be used is the "EMIA-320V" manufactured by Horiba, Ltd.

The content of the (C) inorganic filler in the resin composition is not particularly limited, but is preferably 95% by mass or less, more preferably 90% by mass or less, even more preferably 85% by mass or less, and particularly preferably 80% by mass or less, based on 100% by mass of the non-volatile components in the resin composition. The lower limit of the content of the (C) inorganic filler in the resin composition is not particularly limited, but is preferably 0% by mass or more, 1% by mass or more, and is preferably 5% by mass or more, 10% by mass or more, more preferably 20% by mass or more, 30% by mass or more, even more preferably 40% by mass or more, 50% by mass or more, even more preferably 55% by mass or more, 60% by mass or more, and particularly preferably 65% by mass or more, 70% by mass or more, or 73% by mass or more, based on 100% by mass of the non-volatile components in the resin composition.

The mass ratio of the polycarbonate resin (A) to the inorganic filler (C) in the resin composition (component (A)/component (C)) is not particularly limited, but is preferably 0.001 or more.
The upper limit of the mass ratio of the polycarbonate resin (A) to the inorganic filler (C) in the resin composition (component (A)/component (C)) is not particularly limited, but is preferably 10 or less, more preferably 5 or less, even more preferably 1 or less, and particularly preferably 0.5 or less.

<(D) Epoxy Resin Curing Agent>
The resin composition of the present invention may contain an optional component (D) epoxy resin curing agent. The epoxy resin curing agent (D) may be used alone or in any combination of two or more. The epoxy resin curing agent (D) may have the function of reacting with the epoxy resin (B) to cure it.

(D) Epoxy resin curing agents are not particularly limited, but examples include active ester curing agents, phenolic curing agents, carbodiimide curing agents, acid anhydride curing agents, amine curing agents, benzoxazine curing agents, cyanate ester curing agents, and thiol curing agents. It is particularly preferable that (D) epoxy resin curing agent contains an active ester curing agent.

Active ester curing agents generally include compounds with two or more highly reactive ester groups per molecule, such as phenol esters, thiophenol esters, N-hydroxyamine esters, and esters of heterocyclic hydroxy compounds. These active ester compounds are preferably those obtained by the condensation reaction of a carboxylic acid compound and/or a thiocarboxylic acid compound with a hydroxy compound and/or a thiol compound. From the perspective of improving heat resistance, active ester compounds obtained from a carboxylic acid compound and a hydroxy compound are preferred, and active ester compounds obtained from a carboxylic acid compound and a phenol compound and/or a naphthol compound are more preferred. Examples of carboxylic acid compounds include benzoic acid, acetic acid, succinic acid, maleic acid, itaconic acid, phthalic acid, isophthalic acid, terephthalic acid, and pyromellitic acid. Examples of phenol compounds or naphthol compounds include hydroquinone, resorcinol, bisphenol A, bisphenol F, bisphenol S, phenolphthalene, methylated bisphenol A, methylated bisphenol F, methylated bisphenol S, phenol, o-cresol, m-cresol, p-cresol, catechol, α-naphthol, β-naphthol, 1,5-dihydroxynaphthalene, 1,6-dihydroxynaphthalene, 2,6-dihydroxynaphthalene, dihydroxybenzophenone, trihydroxybenzophenone, tetrahydroxybenzophenone, phloroglucin, benzenetriol, dicyclopentadiene-type diphenol compounds, and phenol novolak. Here, "dicyclopentadiene-type diphenol compounds" refer to diphenol compounds obtained by condensing one dicyclopentadiene molecule with two phenol molecules.

Specific examples of active ester curing agents include dicyclopentadiene-type active ester compounds, naphthalene-type active ester compounds containing a naphthalene structure, active ester compounds containing an acetylated product of phenol novolac, and active ester compounds containing a benzoylated product of phenol novolac. Of these, at least one selected from dicyclopentadiene-type active ester compounds and naphthalene-type active ester compounds is more preferred, with dicyclopentadiene-type active ester compounds being even more preferred. Of the dicyclopentadiene-type active ester compounds, active ester compounds containing a dicyclopentadiene-type diphenol structure are preferred.

Commercially available active ester curing agents include active ester compounds containing a dicyclopentadiene-type diphenol structure, such as "EXB9451," "EXB9460," "EXB9460S," "EXB-8000L," "EXB-8000L-65M," "EXB-8000L-65TM," "HPC-8000L-65TM," "HPC-8000," "HPC-8000-65T," "HPC-8000H," and "HPC-8000H-65TM" (manufactured by DIC Corporation); and active ester compounds containing a naphthalene structure, such as "HP-B-8151-62T," "EXB-8100L-65T," "EXB-8150-60T," and "EXB-8150- 62T," "EXB-9416-70BK," "HPC-8150-60T," "HPC-8150-62T," and "EXB-8" (manufactured by DIC Corporation); a phosphorus-containing active ester compound such as "EXB9401" (manufactured by DIC Corporation); an active ester compound which is an acetylated product of phenol novolac such as "DC808" (manufactured by Mitsubishi Chemical Corporation); active ester compounds which are benzoylated products of phenol novolac such as "YLH1026," "YLH1030," and "YLH1048" (manufactured by Mitsubishi Chemical Corporation); and an active ester compound containing a styryl group and a naphthalene structure such as "PC1300-02-65MA" (manufactured by Air Water Inc.).

As a phenolic curing agent, a phenolic curing agent having a novolac structure is preferred from the viewpoint of heat resistance and water resistance. Furthermore, from the viewpoint of adhesion to the adherend, a nitrogen-containing phenolic curing agent is preferred, and a triazine skeleton-containing phenolic curing agent is more preferred. Of these, a triazine skeleton-containing phenolic novolac resin is preferred from the viewpoint of highly satisfying heat resistance, water resistance, and adhesion. Specific examples of phenolic curing agents include "MEH-7700," "MEH-7810," and "MEH-7851" manufactured by Meiwa Kasei Co., Ltd.; "NHN," "CBN," and "GPH" manufactured by Nippon Kayaku Co., Ltd.; "SN-170," "SN-180," "SN-190," "SN-475," "SN-485," "SN-495," "SN-375," and "SN-395" manufactured by Nippon Steel Chemical & Material Co., Ltd.; and "LA-7052," "LA-7054," "LA-3018," "LA-3018-50P," "LA-1356," "TD2090," and "TD-2090-60M" manufactured by DIC Corporation.

Carbodiimide-based curing agents include curing agents having one or more, preferably two or more, carbodiimide structures in one molecule, such as aliphatic biscarbodiimides such as tetramethylene-bis(t-butylcarbodiimide) and cyclohexane-bis(methylene-t-butylcarbodiimide); aromatic biscarbodiimides such as phenylene-bis(xylylcarbodiimide); and aliphatic polycarbodiimides such as polyhexamethylenecarbodiimide, polytrimethylhexamethylenecarbodiimide, polycyclohexylenecarbodiimide, poly(methylenebiscyclohexylenecarbodiimide), and poly(isophoronecarbodiimide). Examples of polycarbodiimides include aromatic polycarbodiimides such as poly(phenylenecarbodiimide), poly(naphthylenecarbodiimide), poly(tolylenecarbodiimide), poly(methyldiisopropylphenylenecarbodiimide), poly(triethylphenylenecarbodiimide), poly(diethylphenylenecarbodiimide), poly(triisopropylphenylenecarbodiimide), poly(diisopropylphenylenecarbodiimide), poly(xylylenecarbodiimide), poly(tetramethylxylylenecarbodiimide), poly(methylenediphenylenecarbodiimide), and poly[methylenebis(methylphenylene)carbodiimide].

Commercially available carbodiimide curing agents include, for example, "Carbodilite V-02B," "Carbodilite V-03," "Carbodilite V-04K," "Carbodilite V-07," and "Carbodilite V-09" manufactured by Nisshinbo Chemical Inc.; and "Stavaxol P," "Stavaxol P400," and "Hykasil 510" manufactured by Rhein Chemie AG.

Acid anhydride curing agents include those having one or more acid anhydride groups in one molecule, with those having two or more acid anhydride groups in one molecule being preferred. Specific examples of acid anhydride curing agents 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. anhydride, 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), polymeric acid anhydrides such as styrene-maleic acid resins in which styrene and maleic acid are copolymerized, and the like. Commercially available acid anhydride curing agents include "HNA-100," "MH-700," "MTA-15," "DDSA," and "OSA" manufactured by New Japan Chemical Co., Ltd.; "YH-306" and "YH-307" manufactured by Mitsubishi Chemical Corporation; "HN-2200" and "HN-5500" manufactured by Hitachi Chemical Co., Ltd.; and "EF-30," "EF-40," "EF-60," and "EF-80" manufactured by Clay Valley.

Amine-based curing agents include those containing one or more, preferably two or more, amino groups in one molecule. Examples include aliphatic amines, polyether amines, alicyclic amines, and aromatic amines. Of these, aromatic amines are preferred from the perspective of achieving the desired effects of the present invention. Amine-based curing agents are preferably primary or secondary amines, with primary amines being more preferred. Specific examples of amine-based curing agents include 4,4'-methylenebis(2,6-dimethylaniline), 4,4'-diaminodiphenylmethane, 4,4'-diaminodiphenyl sulfone, 3,3'-diaminodiphenyl sulfone, m-phenylenediamine, m-xylylenediamine, diethyltoluenediamine, 4,4'-diaminodiphenyl ether, 3,3'-dimethyl-4,4'-diaminobiphenyl, 2,2'-dimethyl-4,4'-diaminobiphenyl, 3,3'-dihydroxybenzidine, and 2,2-bis(3-amino-4-hydroxyphenyl)propanol. 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, and the like. Commercially available amine-based curing agents may be used, such as "SEIKACURE-S" manufactured by Seika Corporation, "KAYABOND C-200S", "KAYABOND C-100", "KAYAHARD A-A", "KAYAHARD A-B", and "KAYAHARD A-S" manufactured by Nippon Kayaku Co., Ltd., and "Epicure W" manufactured by Mitsubishi Chemical Corporation.

Specific examples of benzoxazine-based curing agents include "JBZ-OP100D" and "ODA-BOZ" manufactured by JFE Chemical Corporation; "HFB2006M" manufactured by Showa Highpolymer Co., Ltd.; and "P-d" and "F-a" manufactured by Shikoku Chemicals Corporation.

Examples of cyanate ester curing agents 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; multifunctional 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 curing agents include Lonza Japan's "PT30" and "PT60" (both phenol novolac-type multifunctional cyanate ester resins), "BA230" and "BA230S75" (prepolymers in which part or all of bisphenol A dicyanate has been triazinated to form a trimer).

Examples of thiol-based curing agents include trimethylolpropane tris(3-mercaptopropionate), pentaerythritol tetrakis(3-mercaptobutyrate), and tris(3-mercaptopropyl)isocyanurate.

The reactive group equivalent of the (D) epoxy resin curing agent is preferably 50 g/eq. to 3000 g/eq., more preferably 100 g/eq. to 1000 g/eq., even more preferably 100 g/eq. to 500 g/eq., and particularly preferably 100 g/eq. to 300 g/eq. The reactive group equivalent is the mass of (D) epoxy resin curing agent per equivalent of reactive groups.

The content of (D) epoxy resin curing agent in the resin composition is not particularly limited, but is preferably 30% by mass or less, more preferably 20% by mass or less, even more preferably 10% by mass or less, and particularly preferably 7% by mass or less, based on 100% by mass of the non-volatile components in the resin composition. The lower limit of the content of (D) epoxy resin curing agent in the resin composition is not particularly limited, but may be, for example, 0% by mass or more, 0.01% by mass or more, 0.1% by mass or more, or 1% by mass or more, preferably 2% by mass or more, more preferably 3% by mass or more, and particularly preferably 4% by mass or more, based on 100% by mass of the non-volatile components in the resin composition.

<(E) Radically Polymerizable Compound>
The resin composition of the present invention may contain a radically polymerizable compound (E) as an optional component. The radically polymerizable compound (E) may be used alone or in any combination of two or more.

In one embodiment, the (E) radical polymerizable compound is a radical polymerizable compound having an ethylenically unsaturated bond. The (E) radical polymerizable compound is not particularly limited, but may have a radical polymerizable group such as an unsaturated hydrocarbon group such as an allyl group, a 3-cyclohexenyl group, a 3-cyclopentenyl group, a 2-vinylphenyl group, a 3-vinylphenyl group, or a 4-vinylphenyl group; or an α,β-unsaturated carbonyl group such as an acryloyl group, a methacryloyl group, or a maleimide group (2,5-dihydro-2,5-dioxo-1H-pyrrol-1-yl group). The (E) radical polymerizable compound preferably has two or more radical polymerizable groups.

In the first embodiment, the (E) radical polymerizable compound preferably includes a thermoplastic resin having a vinylphenyl group and/or a (meth)acryloyl group. The (meth)acryloyl group refers to an acryloyl group or a methacryloyl group. The vinylphenyl group includes a 2-vinylphenyl group, a 3-vinylphenyl group, a 4-vinylphenyl group, or any of these groups in which the aromatic carbon atom is further substituted with one or more alkyl groups. Preferably, there are two or more vinylphenyl groups and/or (meth)acryloyl groups per molecule. Examples of thermoplastic resins include phenoxy resins, polyvinyl acetal resins, polystyrene resins, polyethylene resins, polypropylene resins, polybutadiene resins, polyimide resins, polyamideimide resins, polyetherimide resins, polysulfone resins, polyethersulfone resins, polyphenylene ether resins, polyetheretherketone resins, and polyester resins. In this embodiment, the (E) radical polymerizable compound includes modified resins of these resins having a vinylphenyl group and/or a (meth)acryloyl group.

In the first embodiment, the radical polymerizable compound (E) preferably includes a resin selected from a modified polyphenylene ether resin having a vinylphenyl group and/or a (meth)acryloyl group, and a modified polystyrene resin having a vinylphenyl group and/or a (meth)acryloyl group, and even more preferably includes a modified polyphenylene ether resin having a vinylphenyl group and/or a (meth)acryloyl group, and particularly preferably includes a compound represented by formula (E-1):

[In the formula, R ¹¹ and R ¹² each independently represent an alkyl group; R ¹³ , R ¹⁴ , R ²¹ , R ²² , R ²³ , and R ²⁴ each independently represent a hydrogen atom or an alkyl group; R ³¹ and R ³² each independently represent a vinylphenyl group or a (meth)acryloyl group; Y ¹ represents a single bond, —C(R ^y ) ₂ —, —O—, —CO—, —S—, —SO—, or —SO ₂ —; R ^y each independently represent a hydrogen atom or an alkyl group; Y ² represents a single bond or an alkylene group; p represents 0 or 1; and q and r each independently represent an integer of 1 or greater.]
The q units and r units may be the same or different for each unit.

^R11 and ^R12 each independently represent an alkyl group, preferably a methyl group. ^R13 and ^R14 each independently represent a hydrogen atom or an alkyl group, preferably a hydrogen atom. ^R21 and ^R22 each independently represent a hydrogen atom or an alkyl group, preferably a hydrogen atom or a methyl group, more preferably a methyl group. ^R23 and ^R24 each independently represent a hydrogen atom or an alkyl group, preferably a hydrogen atom or a methyl group.

R ³¹ and R ³² each independently represent a vinylphenyl group or a (meth)acryloyl group, and Y ² represents a single bond or an alkylene group. The alkylene group refers to a linear, branched, and/or cyclic divalent aliphatic saturated hydrocarbon group. The alkylene group is preferably an alkylene group having 1 to 14 carbon atoms, preferably an alkylene group having 1 to 10 carbon atoms, and preferably an alkylene group having 1 to 6 carbon atoms. Examples of the alkylene group include -CH ₂ -, -CH ₂ -CH ₂ -, -CH(CH ₃ ) -, -CH ₂ -CH ₂ -CH ₂ -, -CH ₂ -CH(CH ₃ ) -, -CH(CH ₃ )-CH ₂ -, and -C(CH ₃ ) ₂ -. Preferably, R ³¹ and R ³² are vinylphenyl groups and Y ² is an alkylene group (particularly preferably —CH ₂ —), or R ³¹ and R ³² are (meth)acryloyl groups and Y ² is a single bond.

Y ¹ represents a single bond, -C(R ^y ) ₂ -, -O-, -CO-, -S-, -SO-, or -SO ₂ -, and is preferably a single bond, -C(R ^y ) ₂ -, or -O-. Each R ^y independently represents a hydrogen atom or an alkyl group, and is preferably a hydrogen atom or a methyl group. p represents 0 or 1, and is preferably 1. q and r each independently represent an integer of 1 or more, and are preferably integers of 1 to 200, and more preferably integers of 1 to 100.

Commercially available products of the radically polymerizable compound (E) in the first embodiment include, for example, "OPE-2St 1200" and "OPE-2St 2200" (vinylbenzyl-modified polyphenylene ether resins) manufactured by Mitsubishi Gas Chemical Company, Inc.; and "SA9000" and "SA9000-111" (methacrylic-modified polyphenylene ether resins) manufactured by SABIC Innovative Plastics.

In the second embodiment, the radical polymerizable compound (E) is preferably represented by formula (E-2'):

[In the formula, ring C represents a monocycloalkane ring which may have a substituent, or a monocycloalkene ring which may have a substituent; c and d each independently represent an integer of 0 or 1 or more, and the sum of c and d is 6 or more; and * represents a bonding site.]
The maleimide compound includes a maleimide compound having a partial structure represented by the following formula: The maleimide compound means a compound containing at least one maleimide group (2,5-dihydro-2,5-dioxo-1H-pyrrol-1-yl group) in one molecule. The number of maleimide groups in one molecule of the maleimide compound in the second embodiment is preferably 2 or more, and particularly preferably 2. The maleimide compound in the second embodiment may be used alone or in combination of two or more at any ratio.

The term "monocycloalkane ring" refers to a monocyclic aliphatic saturated hydrocarbon ring. The monocycloalkane ring is preferably a monocycloalkane ring having 4 to 14 carbon atoms, more preferably a monocycloalkane ring having 4 to 10 carbon atoms, and particularly preferably a monocycloalkane ring having 5 or 6 carbon atoms. Examples of monocycloalkane rings include a cyclobutane ring, cyclopentane ring, cyclohexane ring, cycloheptane ring, and cyclooctane ring. The term "monocycloalkene ring" refers to a monocyclic aliphatic unsaturated hydrocarbon ring having at least one carbon-carbon double bond. The monocycloalkene ring is preferably a monocycloalkene ring having 4 to 14 carbon atoms, more preferably a monocycloalkene ring having 4 to 10 carbon atoms, and particularly preferably a monocycloalkene ring having 5 or 6 carbon atoms. Examples of monocycloalkene rings include cyclobutene rings, cyclopentene rings, cyclohexene rings, cycloheptene rings, cyclooctene rings, cyclopentadiene rings, and cyclohexadiene rings.

Ring C represents a monocycloalkane ring which may have a substituent, or a monocycloalkene ring which may have a substituent. Ring C is preferably a monocycloalkane ring which may have a substituent selected from an alkyl group and an alkenyl group; or a monocycloalkene ring which may have a substituent selected from an alkyl group and an alkenyl group. Ring C is more preferably a monocycloalkane ring which may have a substituent selected from an alkyl group having 1 to 14 carbon atoms and an alkenyl group having 2 to 14 carbon atoms; or a monocycloalkene ring which may have a substituent selected from an alkyl group having 1 to 14 carbon atoms and an alkenyl group having 2 to 14 carbon atoms.

c and d each independently represent an integer of 0 or 1 or greater, and the sum of c and d is 6 or greater (preferably 8 or greater, more preferably 10 or greater). Preferably, c and d each independently represent an integer from 0 to 20, and the sum of c and d is 6 or greater (preferably 8 or greater, more preferably 10 or greater). More preferably, c and d each independently represent an integer from 1 to 20, and the sum of c and d is 6 or greater (preferably 8 or greater, more preferably 10 or greater). Even more preferably, c and d each independently represent an integer from 5 to 10. Particularly preferably, c and d are 8.

In the second embodiment, the radical polymerizable compound (E) is particularly preferably a compound represented by formula (E-2):

[In the formula, each ^R5 independently represents a substituent; each D ring independently represents an aromatic ring which may have a substituent; ^{each D1} and ^D2 independently represent a single bond, —C(R ^x ) ₂ —, —O—, —CO—, —S—, —SO—, —SO ₂ —, —CONH—, —NHCO—, —COO—, or —OCO—; each R ^x independently represents a hydrogen atom or an alkyl group; each e independently represents 0 or 1; each f independently represents an integer of 0 or 1 or more; each g independently represents 0, 1, or 2; and each m independently represents an integer of 0 or 1 or more; and the other symbols are as defined above.]
The f unit, g unit, and m unit may be the same or different for each unit.

Rings D each independently represent an aromatic ring which may have a substituent, and preferably a benzene ring which may be substituted with a group selected from an alkyl group. ^{D 1} and D ² each independently represent a single bond, -C(R ^x ) ₂ -, -O-, -CO-, -S-, -SO-, -SO ₂ -, -CONH-, -NHCO-, -COO-, or -OCO-, and preferably a single bond, -C(R ^x ) ₂ -, or -O-. ^{R x} each independently represent a hydrogen atom or an alkyl group, and preferably a hydrogen atom or a methyl group. e each independently represent 0 or 1, and preferably 0. f each independently represent an integer of 0 or 1 or more, and preferably 0, 1, 2, or 3, and more preferably 0, 1, or 2. g each independently represent 0, 1, or 2, and preferably 0. m represents an integer of 0 or 1 or more, and preferably 0.

Formula (D) contained in formula (E-2):

[In the formula, * indicates a binding site; other symbols are as defined above.]
The partial structure represented by the formula (D-1) to (D-3):

[In the formula, * is the same as above.]
Examples of the partial structure include:

Commercially available radically polymerizable compounds (E) in the second embodiment include, for example, "BMI-689," "BMI-1500," "BMI-1700," and "BMI-3000J" manufactured by Designer Molecules, Inc.

In the third embodiment, the radical polymerizable compound (E) is preferably represented by formula (E-3):

[In the formula, R ^6s each independently represent a hydrogen atom or an alkyl group; ring E, ring F, and ring G each independently represent an aromatic ring which may have a substituent; Zs each independently represent a single bond, —C(R ^z ) ₂ —, —O—, —CO—, —S—, —SO—, —SO ₂ —, —CONH—, or —NHCO—; R ^zs each independently represent a hydrogen atom or an alkyl group; s represents an integer of 1 or greater; ts each independently represent 0 or 1; and u's each independently represent 0, 1, 2, or 3.]
The s units and u units may be the same or different for each unit. The maleimide compounds in the third embodiment may be used singly or in combination of two or more types in any ratio.

^R6 each independently represents a hydrogen atom or an alkyl group, preferably a hydrogen atom or a methyl group, and more preferably a hydrogen atom. Ring E, ring F, and ring G each independently represent an aromatic ring which may have a substituent, preferably a benzene ring which may have a substituent, more preferably a benzene ring which may be substituted with a group selected from an alkyl group and an aryl group, and particularly preferably an (unsubstituted) benzene ring.

Each Z independently represents a single bond, -C( ^Rz ) _2- , -O-, -CO-, -S-, -SO-, -SO2-, -CONH-, or -NHCO-, preferably a single bond, -C( ^Rz ) _2- , or -O-, more preferably _{a single bond or -C(Rz)2-} ^, _and particularly preferably a single bond. Each ^Rz independently represents a hydrogen atom or an alkyl group, preferably a hydrogen atom or a methyl group.

s represents an integer of 1 or greater, preferably an integer from 1 to 10. Each t independently represents 0 or 1, preferably 1. Each u independently represents 0, 1, 2, or 3, preferably 0, 1, or 2, more preferably 0 or 1, and particularly preferably 1.

Commercially available examples of the radically polymerizable compound (E) in the third embodiment include "MIR-3000-70MT" and "MIR-5000-60T" manufactured by Nippon Kayaku Co., Ltd.

The (E) radically polymerizable compound may contain any one of the preferred thermoplastic resins included in the first embodiment, the preferred maleimide compounds included in the second embodiment, and the preferred maleimide compounds included in the third embodiment, or may contain two or more of these in combination at any ratio.

The radical polymerizable group equivalent of (E) the radical polymerizable compound is preferably 250 g/eq. to 2500 g/eq., more preferably 300 g/eq. to 1500 g/eq. The radical polymerizable group equivalent of (E) the radical polymerizable compound represents the mass of resin per equivalent of radical polymerizable group.

The weight-average molecular weight (Mw) of the (E) radically polymerizable compound is preferably 300 to 40,000, more preferably 300 to 10,000, and particularly preferably 300 to 7,000. The weight-average molecular weight of the resin can be measured as a polystyrene-equivalent value using gel permeation chromatography (GPC).

The content of the (E) radical polymerizable compound in the resin composition is not particularly limited, but is preferably 30% by mass or less, more preferably 20% by mass or less, even more preferably 10% by mass or less, and particularly preferably 7% by mass or less, based on 100% by mass of the non-volatile components in the resin composition. The lower limit of the content of the (E) radical polymerizable compound in the resin composition is not particularly limited, but is, based on 100% by mass of the non-volatile components in the resin composition, for example, 0% by mass or more, 0.01% by mass or more, preferably 0.1% by mass or more, more preferably 1% by mass or more, even more preferably 3% by mass or more, and particularly preferably 5% by mass or more.

<(F) Curing Accelerator>
The resin composition of the present invention may contain, as an optional component, a curing accelerator (F). The curing accelerator (F) functions as a curing catalyst that accelerates the curing of the epoxy resin (B).

Examples of the (F) curing accelerator include phosphorus-based curing accelerators, urea-based curing accelerators, guanidine-based curing accelerators, imidazole-based curing accelerators, metal-based curing accelerators, and amine-based curing accelerators. The (F) curing accelerator preferably includes an amine-based curing accelerator. One type of (F) curing accelerator may be used alone, or two or more types may be used in combination.

Examples of phosphorus-based curing accelerators include aliphatic phosphonium salts such as tetrabutylphosphonium bromide, tetrabutylphosphonium chloride, tetrabutylphosphonium acetate, tetrabutylphosphonium decanoate, tetrabutylphosphonium laurate, bis(tetrabutylphosphonium)pyromellitate, tetrabutylphosphonium hydrogenhexahydrophthalate, tetrabutylphosphonium 2,6-bis[(2-hydroxy-5-methylphenyl)methyl]-4-methylphenolate, and di-tert-butylmethylphosphonium tetraphenylborate; methyltriphenylphosphonium bromide, ethyltriphenylphosphonium bromide, propyltriphenylphosphonium bromide, butyltriphenylphosphonium bromide, benzyltriphenylphosphonium chloride, and tetraphenylphosphine. aromatic phosphonium salts such as phosphonium bromide, p-tolyltriphenylphosphonium tetra-p-tolylborate, tetraphenylphosphonium tetraphenylborate, tetraphenylphosphonium tetra-p-tolylborate, triphenylethylphosphonium tetraphenylborate, tris(3-methylphenyl)ethylphosphonium tetraphenylborate, tris(2-methoxyphenyl)ethylphosphonium tetraphenylborate, (4-methylphenyl)triphenylphosphonium thiocyanate, tetraphenylphosphonium thiocyanate, and butyltriphenylphosphonium thiocyanate; aromatic phosphine-borane complexes such as triphenylphosphine-triphenylborane; aromatic phosphine-quinone addition products such as triphenylphosphine-p-benzoquinone addition products; tributylphosphine, tri-t Aliphatic phosphines such as tert-butylphosphine, trioctylphosphine, di-tert-butyl(2-butenyl)phosphine, di-tert-butyl(3-methyl-2-butenyl)phosphine and tricyclohexylphosphine; dibutylphenylphosphine, di-tert-butylphenylphosphine, methyldiphenylphosphine, ethyldiphenylphosphine, butyldiphenylphosphine, diphenylcyclohexylphosphine, triphenylphosphine, tri-o-tolylphosphine, tri-m-tolylphosphine, tri-p-tolylphosphine, tris(4-ethylphenyl)phosphine, tris(4-propylphenyl)phosphine, tris(4-isopropylphenyl)phosphine, tris(4-butylphenyl)phosphine, tris(4-tert-butylphenyl)phosphine, tris(2,4-dimethylphenyl)phosphine, Examples of aromatic phosphines include tris(2,5-dimethylphenyl)phosphine, tris(2,6-dimethylphenyl)phosphine, tris(3,5-dimethylphenyl)phosphine, tris(2,4,6-trimethylphenyl)phosphine, tris(2,6-dimethyl-4-ethoxyphenyl)phosphine, tris(2-methoxyphenyl)phosphine, tris(4-methoxyphenyl)phosphine, tris(4-ethoxyphenyl)phosphine, tris(4-tert-butoxyphenyl)phosphine, diphenyl-2-pyridylphosphine, 1,2-bis(diphenylphosphino)ethane, 1,3-bis(diphenylphosphino)propane, 1,4-bis(diphenylphosphino)butane, 1,2-bis(diphenylphosphino)acetylene, and 2,2'-bis(diphenylphosphino)diphenyl ether.

Examples of urea-based curing accelerators include aliphatic dimethylureas such as 1,1-dimethylurea, 1,1,3-trimethylurea, 3-ethyl-1,1-dimethylurea, 3-cyclohexyl-1,1-dimethylurea, and 3-cyclooctyl-1,1-dimethylurea; 3-phenyl-1,1-dimethylurea, 3-(4-chlorophenyl)-1,1-dimethylurea, 3-(3,4-dichlorophenyl)-1,1-dimethylurea, 3-(3-chloro-4-methylphenyl)-1,1-dimethylurea, 3-(2-methylphenyl)-1,1-dimethylurea, 3-(4-methylphenyl)-1,1-dimethylurea, and 3-(3,4-dimethylphenyl)-1,1-dimethylurea. Examples of aromatic dimethylureas include toluene bis(dimethylurea), 3-(4-isopropylphenyl)-1,1-dimethylurea, 3-(4-methoxyphenyl)-1,1-dimethylurea, 3-(4-nitrophenyl)-1,1-dimethylurea, 3-[4-(4-methoxyphenoxy)phenyl]-1,1-dimethylurea, 3-[4-(4-chlorophenoxy)phenyl]-1,1-dimethylurea, 3-[3-(trifluoromethyl)phenyl]-1,1-dimethylurea, N,N-(1,4-phenylene)bis(N',N'-dimethylurea), and N,N-(4-methyl-1,3-phenylene)bis(N',N'-dimethylurea) [toluene bisdimethylurea].

Examples of guanidine-based curing accelerators include dicyandiamide, 1-methylguanidine, 1-ethylguanidine, 1-cyclohexylguanidine, 1-phenylguanidine, 1-(o-tolyl)guanidine, dimethylguanidine, diphenylguanidine, trimethylguanidine, tetramethylguanidine, pentamethylguanidine, 1,5,7-triazabicyclo[4.4.0]dec-5-ene, 7-methyl-1,5,7-triazabicyclo[4.4.0]dec-5-ene, 1-methylbiguanide, 1-ethylbiguanide, 1-n-butylbiguanide, 1-n-octadecylbiguanide, 1,1-dimethylbiguanide, 1,1-diethylbiguanide, 1-cyclohexylbiguanide, 1-allylbiguanide, 1-phenylbiguanide, and 1-(o-tolyl)biguanide.

Examples of imidazole curing accelerators include 2-methylimidazole, 2-undecylimidazole, 2-heptadecylimidazole, 1,2-dimethylimidazole, 2-ethyl-4-methylimidazole, 1,2-dimethylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2-phenyl-4-methylimidazole, 1-benzyl-2-methylimidazole, and 1-benzyl-2- Phenylimidazole, 1-cyanoethyl-2-methylimidazole, 1-cyanoethyl-2-undecylimidazole, 1-cyanoethyl-2-ethyl-4-methylimidazole, 1-cyanoethyl-2-phenylimidazole, 1-cyanoethyl-2-undecylimidazole, 1-cyanoethyl-2-phenylimidazolium trimellitate, 1-cyanoethyl-2-phenylimidazolium trimellitate, 2,4-diamino-6-[2'-methylimidazolyl -(1')]-ethyl-s-triazine, 2,4-diamino-6-[2'-undecylimidazolyl-(1')]-ethyl-s-triazine, 2,4-diamino-6-[2'-ethyl-4'-methylimidazolyl-(1')]-ethyl-s-triazine, 2,4-diamino-6-[2'-methylimidazolyl-(1')]-ethyl-s-triazine isocyanuric acid adduct, 2-phenylimidazole isocyanuric acid adduct Examples include imidazole compounds such as 2-phenyl-4,5-dihydroxymethylimidazole, 2-phenyl-4-methyl-5-hydroxymethylimidazole, 2,3-dihydro-1H-pyrrolo[1,2-a]benzimidazole, 1-dodecyl-2-methyl-3-benzylimidazolium chloride, 2-methylimidazoline, and 2-phenylimidazoline, as well as adducts of imidazole compounds with epoxy resins.

Commercially available imidazole-based curing accelerators may be used, such as "1B2PZ," "2MZA-PW," and "2PHZ-PW" manufactured by Shikoku Chemicals Corporation, and "P200-H50" manufactured by Mitsubishi Chemical Corporation.

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

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

Commercially available amine-based curing accelerators may be used, such as "MY-25" manufactured by Ajinomoto Fine-Techno Co., Ltd.

The content of the (F) curing accelerator in the resin composition is not particularly limited, but is preferably 5% by mass or less, more preferably 1% by mass or less, even more preferably 0.5% by mass or less, and particularly preferably 0.1% by mass or less, based on 100% by mass of the non-volatile components in the resin composition. The lower limit of the content of the (F) curing accelerator in the resin composition is not particularly limited, but may be, for example, 0% by mass or more, 0.001% by mass or more, 0.01% by mass or more, 0.03% by mass or more, based on 100% by mass of the non-volatile components in the resin composition.

<(G) Radical Polymerization Initiator>
The resin composition of the present invention may contain a (G) radical polymerization initiator as an optional component. The (G) radical polymerization initiator may be, for example, a thermal polymerization initiator that generates free radicals upon heating. The (G) radical polymerization initiator may be a polymerization initiator for the radically polymerizable component including the (E) component described above. The (G) radical polymerization initiator may be used alone or in any combination of two or more types.

(G) Examples of radical polymerization initiators include peroxide-based radical polymerization initiators and azo-based radical polymerization initiators. Among these, peroxide-based radical polymerization initiators are preferred.

Peroxide-based radical polymerization initiators include, for example, hydroperoxide compounds such as 1,1,3,3-tetramethylbutyl hydroperoxide; dialkyl peroxide compounds such as tert-butylcumyl peroxide, di-tert-butyl peroxide, di-tert-hexyl peroxide, dicumyl peroxide, 1,4-bis(1-tert-butylperoxy-1-methylethyl)benzene, and 2,5-dimethyl-2,5-bis(tert-butylperoxy)hexane; and diacyl peroxide compounds such as dilauroyl peroxide, didecanoyl peroxide, dicyclohexyl peroxydicarbonate, and bis(4-tert-butylcyclohexyl)peroxydicarbonate. peroxyester compounds such as tert-butyl peroxyacetate, tert-butyl peroxybenzoate, tert-butylperoxyisopropyl monocarbonate, tert-butylperoxy-2-ethylhexanoate, tert-butylperoxyneodecanoate, tert-hexylperoxyisopropyl monocarbonate, tert-butyl peroxylaurate, (1,1-dimethylpropyl) 2-ethylperhexanoate, tert-butyl 2-ethylperhexanoate, tert-butyl 3,5,5-trimethylperhexanoate, tert-butylperoxy-2-ethylhexyl monocarbonate, and tert-butylperoxymaleic acid; and the like.

Examples of azo radical polymerization initiators include azonitrile compounds such as 2,2'-azobis(4-methoxy-2,4-dimethylvaleronitrile), 2,2'-azobis(2,4-dimethylvaleronitrile), 2,2'-azobisisobutyronitrile, 2,2'-azobis(2-methylbutyronitrile), 1,1'-azobis(cyclohexane-1-carbonitrile), 1-[(1-cyano-1-methylethyl)azo]formamide, and 2-phenylazo-4-methoxy-2,4-dimethylvaleronitrile; 2,2'-azobis[2-methyl-N-[1,1-bis(hydroxymethyl)-2-hydroxyethyl]propionamide], 2,2'-azobis[2-methyl-N-[1,1-bis(hydroxymethyl)-2-hydroxyethyl]propionamide], and 2,2'-azobis[2-methyl-N-[1,1-bis(hydroxymethyl)-2-hydroxyethyl]propionamide]. azo amide compounds such as 2,2'-azobis[2-methyl-N-[2-(1-hydroxybutyl)]-propionamide], 2,2'-azobis[2-methyl-N-(2-hydroxyethyl)-propionamide], 2,2'-azobis(2-methylpropionamide) dihydrate, 2,2'-azobis[N-(2-propenyl)-2-methylpropionamide], 2,2'-azobis(N-butyl-2-methylpropionamide), and 2,2'-azobis(N-cyclohexyl-2-methylpropionamide); alkyl azo compounds such as 2,2'-azobis(2,4,4-trimethylpentane) and 2,2'-azobis(2-methylpropane); and the like.

(G) Commercially available radical polymerization initiators include, for example, NOF Corporation's "Perbutyl C," "Perbutyl A," "Perbutyl P," "Perbutyl L," "Perbutyl O," "Perbutyl ND," "Perbutyl Z," "Perbutyl I," "Percumyl P," "Percumyl D," "Perhexyl D," "Perhexyl A," "Perhexyl I," "Perhexyl Z," "Perhexyl ND," "Perhexyl O," and "Perhexyl PV."

The content of the (G) radical polymerization initiator in the resin composition is not particularly limited, but is preferably 1% by mass or less, more preferably 0.5% by mass or less, even more preferably 0.1% by mass or less, and particularly preferably 0.05% by mass or less, based on 100% by mass of the non-volatile components in the resin composition. The lower limit of the content of the (G) radical polymerization initiator in the resin composition is not particularly limited, but is, based on 100% by mass of the non-volatile components in the resin composition, for example, 0% by mass or more, 0.0001% by mass or more, preferably 0.001% by mass or more, more preferably 0.005% by mass or more, even more preferably 0.01% by mass or more, and particularly preferably 0.02% by mass or more.

<(H) Other Additives>
The resin composition of the present invention may further contain any additives as a non-volatile component. Examples of such additives include thermosetting resins other than epoxy resins, such as epoxy acrylate resins, urethane acrylate resins, urethane resins, cyanate resins, benzoxazine resins, unsaturated polyester resins, phenolic resins, melamine resins, and silicone resins; thermoplastic resins, such as phenoxy resins, polyvinyl acetal resins, polyolefin resins, polysulfone resins, polyethersulfone resins, polyphenylene ether resins, polycarbonate resins, polyetheretherketone resins, and polyester resins; organic fillers, such as rubber particles; organometallic compounds, such as organocopper compounds, organozinc compounds, and organocobalt 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-based leveling agents and acrylic polymer-based leveling agents; thickeners, such as bentone and montmorillonite; and silicones. defoaming agents such as benzotriazole-based ultraviolet absorbers; adhesion improvers such as urea silanes; adhesion improvers such as triazole-based adhesion imparters, tetrazole-based adhesion imparters, and triazine-based adhesion imparters; antioxidants such as hindered phenol-based antioxidants; fluorescent brighteners such as stilbene derivatives; surfactants such as fluorine-based surfactants and silicone-based surfactants; phosphorus-based flame retardants (e.g., phosphate ester compounds, phosphazene compounds, Examples of the flame retardants include flame retardants such as 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-based dispersants, polyoxyalkylene-based dispersants, acetylene-based dispersants, silicone-based dispersants, anionic dispersants, and cationic dispersants; and 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. (H) Other additives may be used singly or in combination of two or more in any ratio. The content of (H) Other additives can be appropriately determined by a person skilled in the art.

<(I) Organic Solvent>
The resin composition of the present invention may further contain an arbitrary organic solvent as a volatile component in addition to the non-volatile components described above. (I) As the organic solvent, any known organic solvent can be used appropriately, and the type thereof is not particularly limited. (I) 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, diphenyl ether, and anisole; 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 methoxypropionic acid. Examples of the organic solvent include ether ester solvents such as methyl 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. (I) The organic solvent may be used alone or in combination of two or more in any ratio.

In one embodiment, the content of (I) organic solvent is not particularly limited, but may be, for example, 60% by mass or less, 40% by mass or less, 30% by mass or less, 20% by mass or less, 15% by mass or less, 10% by mass or less, etc., when all components in the resin composition are taken as 100% by mass.

<Method of producing resin composition>
The resin composition of the present invention can be produced, for example, by adding (A) polycarbonate resin, (B) epoxy resin, optionally (C) inorganic filler, optionally (D) epoxy resin curing agent, optionally (E) radical polymerizable compound, optionally (F) curing accelerator, optionally (G) radical polymerization initiator, optionally (H) other additives, and optionally (I) organic solvent to any preparation vessel in any order and/or simultaneously in part or in whole, and mixing. Furthermore, during the process of adding and mixing each component, the temperature can be appropriately set, and heating and/or cooling may be performed temporarily or throughout. Furthermore, during or after the process of adding and mixing, the resin composition may be stirred or shaken using a stirring or shaking device such as a mixer to uniformly disperse the resin composition. Furthermore, degassing may be performed under low-pressure conditions, such as under vacuum, simultaneously with stirring or shaking.

<Characteristics of Resin Composition>
The resin composition of the present invention comprises (A) a polycarbonate resin and (B) an epoxy resin, wherein the component (A) comprises a polycarbonate resin having a repeating structural unit represented by formula (A1). By using such a resin composition, a cured product having a lower dielectric constant (Dk) can be obtained.

The cured product of the resin composition of the present invention may be characterized by a low dielectric constant (Dk). Therefore, in one embodiment, the dielectric constant (Dk) of the cured product of the resin composition, when measured at 5.8 GHz and 23°C as in Test Example 1 below, may be preferably 5.0 or less, more preferably 4.0 or less, even more preferably 3.7 or less, even more preferably 3.5 or less, 3.3 or less, and particularly preferably 3.1 or less, 3.0 or less.

In one embodiment, the cured product of the resin composition of the present invention may be characterized by a low dielectric dissipation factor (Df). Therefore, in one embodiment, the dielectric dissipation factor (Df) of the cured product of the resin composition, measured at 5.8 GHz and 23°C as in Test Example 1 below, may be preferably 0.0100 or less, 0.0080 or less, more preferably 0.0070 or less, 0.0060 or less, even more preferably 0.0050 or less, 0.0045 or less, and particularly preferably 0.0040 or less, 0.0035 or less.

In one embodiment, a cured product of the resin composition of the present invention may be characterized by suppressed warping. Therefore, in one embodiment, the amount of warping measured as in Test Example 2 below may preferably be less than 1 cm.

In one embodiment, the cured product of the resin composition of the present invention may be characterized by excellent copper foil adhesion. Therefore, in one embodiment, the copper foil adhesion strength, measured as in Test Example 3 below, may be preferably 0.2 kgf/cm or more, more preferably 0.25 kgf/cm or more, 0.3 kgf/cm or more, even more preferably 0.35 kgf/cm or more, 0.4 kgf/cm or more, and particularly preferably 0.43 kgf/cm or more, 0.45 kgf/cm or more.

<Uses of resin composition>
The resin composition of the present invention can be suitably used as a resin composition for insulating applications, particularly as a resin composition for forming an insulating layer. Specifically, it can be suitably used as a resin composition for forming an insulating layer (resin composition for forming an insulating layer) for forming a conductor layer (including a rewiring layer) formed on the insulating layer. In addition, it can be suitably used as a resin composition for forming an insulating layer of a printed wiring board (resin composition for forming an insulating layer of a printed wiring board) in the printed wiring board described below. 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, underfill materials, die bonding materials, semiconductor encapsulants, hole-filling resins, and component embedding resins.

Furthermore, for example, when a semiconductor chip package is manufactured through the following steps (1) to (6), the resin composition of the present invention can be suitably used as a resin composition for a rewiring formation layer (resin composition for forming a rewiring formation layer) as an insulating layer for forming a rewiring layer, and as a resin composition for encapsulating a semiconductor chip (resin composition for encapsulating a semiconductor chip). When a semiconductor chip package is manufactured, a rewiring layer may be further formed on the encapsulation layer.
(1) A step of laminating a temporary fixing film on 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) forming a rewiring layer as a conductor layer on the rewiring formation layer.

In addition, the resin composition of the present invention provides an insulating layer with good component embedding properties, making it suitable for use in printed wiring boards that are circuit boards with built-in components.

<Sheet-shaped laminated material>
The resin composition of the present invention can be used by applying it in the form of a varnish, but industrially it is generally preferred to use it in the form of a sheet-like laminate material containing the resin composition.

The following resin sheets and prepregs are preferred as sheet-like laminate materials.

In one embodiment, the resin sheet comprises a support and a resin composition layer provided on the support, and the resin composition layer is formed from the resin composition of the present invention.

The thickness of the resin composition layer is preferably 50 μm or less, more preferably 40 μm or less, from the viewpoint of making printed wiring boards thinner and being able to provide a cured product of the resin composition that has excellent insulating properties even when the cured product is thin. There is no particular lower limit to the thickness of the resin composition layer, but it can usually be 5 μm or more, 10 μm or more, etc.

Examples of the support include films made of plastic materials, metal foils, and release paper, with films made of plastic materials and metal foils being preferred.

When a film made of a plastic material is used as the support, examples of the plastic material include polyesters such as polyethylene terephthalate (hereinafter sometimes abbreviated as "PET") and polyethylene naphthalate (hereinafter sometimes abbreviated as "PEN"), polycarbonate (hereinafter sometimes abbreviated as "PC"), acrylics such as polymethyl methacrylate (PMMA), cyclic polyolefins, triacetyl cellulose (TAC), polyether sulfide (PES), polyether ketone, polyimide, etc. Among these, polyethylene terephthalate and polyethylene naphthalate are preferred, with inexpensive polyethylene terephthalate being particularly preferred.

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

The surface of the support that will be bonded to the resin composition layer may be subjected to a matte finish, corona treatment, or antistatic treatment.

The support may also be a support with a release layer, which has a release layer on the surface that bonds with the resin composition layer. Examples of release agents used in the release layer of the support with a release layer include one or more release agents selected from the group consisting of alkyd resins, polyolefin resins, urethane resins, and silicone resins. Commercially available products may be used as the support with a release layer, including PET films with a release layer primarily composed of an alkyd resin-based release agent, such as "SK-1," "AL-5," and "AL-7" manufactured by Lintec Corporation, "Lumirror T60" manufactured by Toray Industries, Inc., "Purex" manufactured by Teijin Limited, and "Uni-Peel" manufactured by Unitika Ltd.

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 using a support with a release layer, it is preferable that the overall thickness of the support with a release layer be in the above range.

In one embodiment, the resin sheet may further include an optional layer, if necessary. Examples of such optional layers include a protective film conforming to the support, provided on the surface of the resin composition layer that is not bonded to the support (i.e., the surface opposite the support). The thickness of the protective film is not particularly limited, but is, for example, 1 μm to 40 μm. By laminating a protective film, it is possible to prevent the adhesion of dust and other particles to the surface of the resin composition layer and to prevent scratches.

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

The organic solvent may be the same as the organic solvents described as components of the resin composition. One organic solvent may be used alone, or two or more organic solvents may be used in combination.

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

The resin sheet can be stored rolled up. If the resin sheet has a protective film, it can be used by peeling off the protective film.

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

The sheet-like fiber substrate used for the prepreg is not particularly limited, and commonly used prepreg substrates such as glass cloth, aramid nonwoven fabric, and liquid crystal polymer nonwoven fabric can be used. From the perspective of thinning the printed wiring board, 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. There is no particular lower limit to the thickness of the sheet-like fiber substrate. It is usually 10 μm or more.

Prepregs can be manufactured using known methods such as the hot melt method and the solvent method.

The thickness of the prepreg can be in the same range as the resin composition layer in the resin sheet described above.

The sheet-like laminate material of the present invention can be suitably used to form insulating layers in printed wiring boards (for insulating layers in printed wiring boards), and can be even more suitably used to form interlayer insulating layers in printed wiring boards (for interlayer insulating layers in printed wiring boards).

<Printed wiring board>
The printed wiring board of the present invention includes an insulating layer made of a cured product obtained by curing the resin composition of the present invention.

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 so that the resin composition layer of the resin sheet is bonded to the inner layer substrate; and (II) a step of curing (e.g., thermally curing) the resin composition layer to form an insulating layer.

The "inner layer substrate" used in step (I) refers to a component that will become the substrate of a printed wiring board, and examples include glass epoxy substrates, metal substrates, polyester substrates, polyimide substrates, BT resin substrates, and thermosetting polyphenylene ether substrates. The substrate may also have a conductor layer on one or both sides, and this conductor layer may be patterned. An inner layer substrate with a conductor layer (circuit) formed on one or both sides of the substrate is sometimes referred to as an "inner layer circuit board." Furthermore, the term "inner layer substrate" used in this invention also includes intermediate products on which insulating layers and/or conductor layers are to be further formed during the manufacture of a printed wiring board. When the printed wiring board is a component-embedded circuit board, an inner layer substrate with embedded components may be used.

The inner layer substrate and resin sheet can be laminated, for example, by thermocompression bonding the resin sheet to the inner layer substrate from the support side. Examples of the member that thermocompresses the resin sheet to the inner layer substrate (hereinafter also referred to as the "thermocompression member") include a heated metal plate (such as a SUS panel) or a metal roll (SUS roll). It is preferable to press the thermocompression member not directly onto the resin sheet, but rather via an elastic material such as heat-resistant rubber, so that the resin sheet can adequately conform to the surface irregularities of the inner layer substrate.

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

Lamination can be performed using a commercially available vacuum laminator. Examples of commercially available vacuum laminators include the vacuum pressure laminator manufactured by Meiki Seisakusho Co., Ltd., the vacuum applicator manufactured by Nikko Materials Co., Ltd., and the batch vacuum pressure laminator.

After lamination, the laminated resin sheets may be smoothed under normal pressure (atmospheric pressure), for example, by pressing a thermocompression member from the support side. The pressing conditions for the smoothing process may be the same as the thermocompression conditions for lamination described above. The smoothing process may be performed using a commercially available laminator. Note that lamination and smoothing may also be performed consecutively using the commercially available vacuum laminator described above.

The support may be removed between steps (I) and (II), or after step (II).

In step (II), the resin composition layer is cured (e.g., thermally cured) to form an insulating layer made of the cured resin composition. The curing conditions for the resin composition layer are not particularly limited, and conditions typically used for forming insulating layers for printed wiring boards may be used.

For example, the thermal curing conditions for the resin composition layer vary depending on the type of resin composition, but in one embodiment, the curing temperature is preferably 120°C to 240°C, more preferably 150°C to 220°C, and even more preferably 170°C to 210°C. The curing time is preferably 5 to 120 minutes, more preferably 10 to 100 minutes, and even more preferably 15 to 100 minutes.

Before thermally curing the resin composition layer, 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 120°C, preferably 60°C to 115°C, and more preferably 70°C to 110°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.

When manufacturing a printed wiring board, the following steps may be further carried out: (III) drilling holes in the insulating layer; (IV) roughening the insulating layer; and (V) forming a conductor layer. These steps (III) through (V) may be carried out according to various methods known to those skilled in the art and used in the manufacture of printed wiring boards. If the support is removed after step (II), the removal of the support may be carried out between steps (II) and (III), between steps (III) and (IV), or between steps (IV) and (V). If necessary, the formation of the insulating layer and conductor layer in steps (II) through (V) may be repeated to form a multilayer wiring board.

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

Step (III) is a step of drilling holes in the insulating layer, thereby forming holes such as via holes and through holes in the insulating layer. Step (III) may be performed using, for example, a drill, 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 determined appropriately depending on the design of the printed wiring board.

Step (IV) is a step in which the insulating layer is roughened. Typically, smear removal is also performed in this step (IV). The roughening treatment procedures and conditions are not particularly limited, and known procedures and conditions commonly used in forming insulating layers for printed wiring boards can be used. For example, the insulating layer can be roughened by performing a swelling treatment using a swelling liquid, a roughening treatment using an oxidizing agent, and a neutralization treatment using a neutralizing liquid, in that order.

The swelling liquid used in the roughening treatment is not particularly limited, but examples include alkaline solutions and surfactant solutions. Alkaline solutions are preferred, with sodium hydroxide and potassium hydroxide solutions being more preferred. Commercially available swelling liquids include "Swelling Dip Securigans P" and "Swelling Dip Securigans SBU" manufactured by Atotech Japan. The swelling treatment using a swelling liquid is not particularly limited, but can be carried out by immersing the insulating layer in a swelling liquid at 30°C to 90°C for 1 to 20 minutes, for example. To keep swelling of the resin in 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.

The oxidizing agent used in the roughening treatment is not particularly limited, but examples include alkaline permanganate solutions prepared by dissolving potassium permanganate or sodium permanganate in an aqueous solution of sodium hydroxide. Roughening treatment using an oxidizing agent such as alkaline permanganate solution is preferably carried out by immersing the insulating layer in an oxidizing agent solution heated to 60°C to 100°C for 10 to 30 minutes. The concentration of permanganate in the alkaline permanganate solution is preferably 5% to 10% by mass. Commercially available oxidizing agents include alkaline permanganate solutions such as "Concentrate Compact CP" and "Dosing Solution Securigance P" manufactured by Atotech Japan.

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 is one example.

Treatment with a 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 standpoint of workability, etc., it is preferable to immerse the object that has been roughened with an oxidizing agent in a neutralizing solution at 40°C to 70°C for 5 to 20 minutes.

In one embodiment, the arithmetic mean roughness (Ra) of the insulating layer surface after the roughening treatment is not particularly limited, but is preferably 500 nm or less, more preferably 400 nm or less, and even more preferably 300 nm or less. The lower limit is not particularly limited, and may be, for example, 1 nm or more, 2 nm or more, etc. Furthermore, the root mean square roughness (Rq) of the insulating layer surface after the roughening treatment is preferably 500 nm or less, more preferably 400 nm or less, and even more preferably 300 nm or less. The lower limit is not particularly limited, and may be, for example, 1 nm or more, 2 nm or more, etc. The arithmetic mean roughness (Ra) and root mean square roughness (Rq) of the insulating layer surface can be measured using a non-contact surface roughness meter.

Step (V) is a step of forming a conductor layer, in which 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. Examples of alloy layers include layers formed from alloys of two or more metals selected from the above group (e.g., nickel-chromium alloys, copper-nickel alloys, and copper-titanium alloys). Among these, from the standpoint of versatility in forming the conductor layer, cost, ease of patterning, etc., 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.

The conductor layer may have a single-layer structure, or a multi-layer structure consisting of two or more single-metal or alloy layers made of different types of metals or alloys. If 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 nickel-chromium alloy.

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

In one embodiment, the conductor layer may be formed by plating. For example, a conductor layer having a desired wiring pattern can be formed by plating the surface of the insulating layer using conventional techniques such as semi-additive and full-additive methods. From the perspective of ease of manufacturing, formation by a semi-additive method is preferred. Below is an example of forming a conductor layer by a semi-additive method.

First, a plating seed layer is formed on the surface of the insulating layer by electroless plating. Next, a mask pattern is formed on the formed plating seed layer, exposing a portion of the plating seed layer corresponding to the desired wiring pattern. A metal layer is formed on the exposed plating seed layer by electrolytic plating, and the mask pattern is then removed. Unnecessary plating seed layer is then removed by etching or other methods, forming a conductor layer with the desired wiring pattern.

In another embodiment, the conductor layer may be formed using metal foil. When forming the conductor layer using metal foil, it is preferable to perform step (V) between steps (I) and (II). For example, after step (I), the support is removed and metal foil is laminated on the exposed surface of the resin composition layer. The resin composition layer and metal foil may be laminated using a vacuum lamination method. The lamination conditions may be the same as those described for step (I). Next, step (II) is performed to form an insulating layer. Thereafter, a conductor layer having the desired wiring pattern can be formed using the metal foil on the insulating layer using conventional techniques such as a subtractive method or a modified semi-additive method.

Metal foil can be manufactured by known methods such as electrolysis and rolling. Commercially available metal foils include HLP foil and JXUT-III foil manufactured by JX Nippon Mining & Metals Corporation, and 3EC-III foil and TP-III foil manufactured by Mitsui Mining & Smelting Co., Ltd.

<Semiconductor Device>
The semiconductor device of the present invention includes the printed wiring board of the present invention. The semiconductor device of the present invention can be manufactured using the printed wiring board of the present invention.

Semiconductor devices include various semiconductor devices used in electrical appliances (e.g., computers, mobile phones, digital cameras, and televisions) and vehicles (e.g., motorcycles, automobiles, trains, ships, and aircraft).

The present invention will be explained in more detail below using examples. The present invention is not limited to these examples. In the following, "parts" and "%" used to express amounts refer to "parts by mass" and "% by mass," respectively, unless otherwise specified. Unless otherwise specified, the temperature and pressure conditions are room temperature (23°C) and atmospheric pressure (1 atm), respectively.

Example 1: Preparation of resin composition 1
40 parts of a polycarbonate oligomer ("Ph-PCO-BPCDE" manufactured by Honshu Chemical Industry Co., Ltd., weight-average molecular weight 4080, hydroxyl group content 0.01 mmol/g, main component: polycarbonate resin having a repeating structural unit represented by the following formula (A)), 10 parts of a bixylenol-type epoxy resin ("YX4000H" manufactured by Mitsubishi Chemical Corporation, epoxy equivalent approximately 190 g/eq.), and 5 parts of a bisphenol A-type epoxy resin ("828US" manufactured by Mitsubishi Chemical Corporation, epoxy equivalent approximately 180 g/eq.) were heated and dissolved in 60 parts of MEK with stirring. After cooling to room temperature, 32 parts of an active ester curing agent (DIC Corporation's "HPC-8150-62T," active ester group equivalent weight approximately 220 g/eq., nonvolatile content 62% by mass in toluene solution), 4 parts of a curing accelerator (4-dimethylaminopyridine (DMAP), MEK solution with a solid content of 5% by mass), and 225 parts of spherical silica (Admatechs Co., Ltd.'s "SO-C2," specific surface area 5.9 m ² /g, average particle size 0.77 μm) surface-treated with N-phenyl-8-aminooctyl-trimethoxysilane (Shin-Etsu Chemical Co., Ltd., molecular weight 325.2) were mixed and uniformly dispersed using a high-speed rotary mixer, followed by filtration using a cartridge filter (ROKITECHNO Corporation's "SHP020") to prepare Resin Composition 1 (resin varnish).

Example 2: Preparation of resin composition 2
In Example 1, 32 parts of the active ester curing agent ("HPC-8150-62T" manufactured by DIC Corporation, active ester group equivalent weight: approximately 220 g/eq., non-volatile content: 62% by mass in toluene solution) was changed to 31 parts of an active ester curing agent ("HPC-8000-65T" manufactured by DIC Corporation, active ester group equivalent weight: approximately 223 g/eq., non-volatile content: 65% by mass in toluene solution). Resin composition 2 (resin varnish) was prepared in the same manner as in Example 1, except for the above-mentioned points.

Example 3: Preparation of resin composition 3
In Example 1, the amount of polycarbonate oligomer ("Ph-PCO-BPCDE", manufactured by Honshu Chemical Industry Co., Ltd., weight average molecular weight 4080, hydroxyl group content 0.01 mmol/g) was changed from 40 parts to 200 parts. Resin composition 3 (resin varnish) was prepared in the same manner as in Example 1 except for the above.

Example 4: Preparation of resin composition 4
In Example 1,
1) The amount of spherical silica ("SO-C2", manufactured by Admatechs Co., Ltd., specific surface area 5.9 ^{m 2} /g, average particle size 0.77 μm) surface-treated with N-phenyl-8-aminooctyl-trimethoxysilane (manufactured by Shin-Etsu Chemical Co., Ltd., molecular weight 325.2) was changed from 225 parts to 290 parts,
2) 29 parts of biphenylaralkyl novolac maleimide ("MIR-3000-70MT" manufactured by Nippon Kayaku Co., Ltd., MEK/toluene mixed solution with a non-volatile content of 70%) was added,
3) 0.5 parts of a polymerization initiator (NOF Corporation's "Perhexyl D", an MEK solution with a solid content of 20% by mass) was added.
Resin composition 4 (resin varnish) was prepared in the same manner as in Example 1 except for the above.

Example 5: Preparation of resin composition 5
In Example 4, 29 parts of biphenylaralkyl novolac maleimide ("MIR-3000-70MT" manufactured by Nippon Kayaku Co., Ltd., MEK/toluene mixed solution with a non-volatile content of 70%) was changed to 20 parts of a maleimide liquid curing agent ("BMI689" manufactured by Designer Molecules, Inc., maleimide group equivalent: 345 g/eq.). Resin composition 5 (resin varnish) was prepared in the same manner as in Example 4, except for the above points.

Example 6: Preparation of resin composition 6
In Example 4, 29 parts of biphenylaralkyl novolac maleimide ("MIR-3000-70MT" manufactured by Nippon Kayaku Co., Ltd., MEK/toluene mixed solution with a non-volatile content of 70%) was changed to 20 parts of methacrylic-modified polyphenylene ether ("SA9000-111" manufactured by SABIC Innovative Plastics). Resin composition 6 (resin varnish) was prepared in the same manner as in Example 4 except for the above.

Example 7: Preparation of resin composition 7
In Example 4, 29 parts of biphenylaralkyl novolac maleimide ("MIR-3000-70MT" manufactured by Nippon Kayaku Co., Ltd., MEK/toluene mixed solution with a non-volatile content of 70%) was changed to 31 parts of vinylbenzyl-modified polyphenylene ether ("OPE-2St 2200" manufactured by Mitsubishi Gas Chemical Co., Ltd., toluene solution with a non-volatile content of 65%). Resin composition 7 (resin varnish) was prepared in the same manner as in Example 4, except for the above-mentioned points.

Comparative Example 1: Preparation of Resin Composition 8
In Example 1, 40 parts of polycarbonate oligomer ("Ph-PCO-BPCDE" manufactured by Honshu Chemical Industry Co., Ltd., weight average molecular weight 4080, hydroxyl group content 0.01 mmol/g) was changed to 40 parts of polycarbonate ("FPC2136" manufactured by Mitsubishi Gas Chemical Co., Ltd., weight average molecular weight 20895, main component: polycarbonate resin having repeating structural units represented by the following formula (A'-1) and repeating structural units represented by the following formula (A'-2)). Resin composition 8 (resin varnish) was prepared in the same manner as in Example 1, except for the above details.

<Test Example 1: Measurement and Evaluation of Relative Dielectric Constant (Dk) and Dielectric Loss Tangent (Df)>
(1) Preparation of a resin sheet having a resin composition layer thickness of 40 μm A polyethylene terephthalate film ("AL5" manufactured by Lintec Corporation, thickness 38 μm) with a release layer was prepared as a support. The resin compositions obtained in the examples and comparative examples were uniformly applied to the release layer of this support so that the thickness of the resin composition layer after drying would be 40 μm. The resin composition was then dried at 80°C to 100°C (average 90°C) for 4 minutes to obtain a resin sheet including a support and a resin composition layer.

(2) Preparation of Cured Product for Evaluation The resin sheet obtained in (1) above was cured in an oven at 200°C for 90 minutes. The resin sheet was removed from the oven and the support was peeled off to obtain a cured product of the resin composition layer. The cured product was cut into a length of 80 mm and a width of 2 mm to prepare a cured product for evaluation.

(3) Measurement of relative permittivity and dielectric loss tangent The values of relative permittivity (Dk) and dielectric loss tangent (Df) of the cured product for evaluation obtained in (2) above were measured by the cavity resonance perturbation method using a cavity resonator perturbation dielectric constant measuring device "CP521" manufactured by Kanto Applied Electronics Development Co., Ltd. and an "HP8362B" manufactured by Agilent Technologies at a measurement frequency of 5.8 GHz and a measurement temperature of 23°C. Measurements were carried out on three test pieces, and the average was calculated and evaluated according to the following evaluation criteria.

Evaluation criteria: "◯": When the relative dielectric constant is 3.1 or less and the dielectric loss tangent is 0.0040 or less; "×": When the relative dielectric constant is more than 3.1 or the dielectric loss tangent is more than 0.0040.

<Test Example 2: Measurement and Evaluation of Warpage>
(1) Lamination of Resin Sheet A resin sheet prepared in the same manner as in Test Example 1 (1) was cut into a size of 9.5 cm square and laminated onto the roughened surface of a 10 cm square Mitsui Mining & Smelting copper foil "3EC-III (thickness 35 μm)" cut into a 10 cm square using a batch-type vacuum pressure laminator (Nikko Materials Co., Ltd., two-stage build-up laminator, CVP700). The laminate was prepared by reducing the pressure for 30 seconds to 13 hPa or less, and then pressing at 120 ° C. for 30 seconds at a pressure of 0.74 MPa to produce a metal foil with a resin composition layer, and then peeling off the PET film.

(2) Curing of Resin Composition Layer The four sides of the metal foil with the resin composition layer obtained in (1) above were attached to a 1 mm thick SUS plate with polyimide tape so that the resin composition layer was on top, and the resin composition layer was cured under curing conditions of 190°C and 90 minutes.

(3) Measurement of Warpage The polyimide tape was peeled off from three of the four sides of the metal foil with the resin composition layer obtained in (2) above, and the height of the highest point from the SUS plate was measured to determine the warpage value. The magnitude of the warpage was evaluated according to the following criteria.
"Good": The size of the warp is less than 1 cm. "Good": The size of the warp is 1 cm or more but less than 3 cm. "Poor": The size of the warp is 3 cm or more.

<Test Example 3: Measurement and Evaluation of Copper Foil Adhesion>
(1) Copper Foil Primer Treatment The shiny side of "3EC-III" (electrolytic copper foil, 35 μm) manufactured by Mitsui Mining & Smelting Co., Ltd. was etched to a depth of 1 μm with a microetching agent ("CZ8101" manufactured by MEC Co., Ltd.) to roughen the copper surface, and then an anti-rust treatment (CL8300) was applied. Furthermore, the foil was heated in an oven at 130° C. for 30 minutes. This copper foil is referred to as CZ copper foil.

(2) Preparation of Inner Layer Substrate 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") on which an inner layer circuit had been formed were etched by 1 μm with a microetching agent (MEC "CZ8101") to roughen the copper surface.

(3) Lamination of Copper Foil and Formation of Insulating Layer The protective film was peeled off from the resin sheet prepared in the same manner as in Test Example 1 (1) to expose the resin composition layer. Using a batch-type vacuum pressure laminator (Nikko Materials Co., Ltd., two-stage build-up laminator "CVP700"), the resin composition layer was laminated on both sides of the inner layer substrate prepared in (2) above so that it was in contact with the inner layer substrate. 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 onto the resin composition layer under the same conditions as above. Then, the resin composition layer was cured at 200 ° C. for 90 minutes to form an insulating layer, thereby producing an evaluation substrate.

(4) Measurement of Copper Foil Adhesion The evaluation substrate prepared in (3) above 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) when 35 mm was peeled off vertically at a rate of 50 mm/min at room temperature was measured to determine the peel strength. A tensile tester ("AC-50C-SL" manufactured by TSE Corporation) was used for the measurement. The measurement was performed in accordance with Japanese Industrial Standards (JIS C6481), and the copper foil adhesion (adhesion strength) was evaluated according to the following criteria.
"Good": Adhesion strength is 0.40 kgf/cm or more "Poor": Adhesion strength is less than 0.40 kgf/cm

The non-volatile component contents of the resin compositions of the Examples and Comparative Examples, as well as the measurement results and evaluation results of the test examples, are shown in Table 1 below.

As shown in Table 1, by using a resin composition containing (A) a polycarbonate resin and (B) an epoxy resin, where component (A) contains a polycarbonate resin having a repeating structural unit represented by formula (A1) described above, it is possible to obtain a cured product with a lower relative dielectric constant (Dk). Furthermore, it is clear that such a cured product has a low dielectric dissipation factor (Df), reduced warpage, and high copper foil adhesion.

Claims (13)

A resin composition comprising (A) a polycarbonate resin, (B) an epoxy resin, and (C) an inorganic filler,
The component (A) is represented by the formula (A1):
[In the formula,
Ring A and ring B each independently represent an aromatic ring which may have a substituent;
Ring X represents a non-aromatic carbocyclic ring having 7 or more carbon atoms which may have a substituent.
The polycarbonate resin contains a repeating structural unit represented by
The weight average molecular weight of the component (A) is 3,000 or more,
The hydroxyl group content of component (A) is 0.05 mmol/g or less,
The content of the component (A) is 10% by mass or more and 50% by mass or less, when the total amount of non-volatile components in the resin composition is 100% by mass,
The content of the (B) component is 3% by mass or more and 20% by mass or less, when the total amount of non-volatile components in the resin composition is 100% by mass,
The content of the component (C) is 40% by mass or more and 80% by mass or less, when the total amount of nonvolatile components in the resin composition is 100% by mass,
the total content of the (A) component, the (B) component, and the (C) component is 73% by mass or more and 98% by mass or less,
the mass ratio of the polycarbonate resin (A) to the inorganic filler (C) (component (A)/component (C)) is 0.1 or more and 1 or less,
the dielectric loss tangent (Df) of a cured product of the resin composition is 0.0040 or less when measured at 5.8 GHz and 23°C;
A resin composition, wherein the relative dielectric constant (Dk) of a cured product of the resin composition is 3.1 or less when measured at 5.8 GHz and 23°C. The component (A) is a compound represented by the formula (A3):
[In the formula,
R ¹ and R ² each independently represent a hydrogen atom, an alkyl group, or an aryl group;
^R3 and ^R4 each independently represent an alkyl group or an aryl group;
a and b each independently represent 0, 1, 2, 3, or 4;
n represents an integer of 6 or more.
The resin composition according to claim 1, comprising a polycarbonate resin having a repeating structural unit represented by the formula: The resin composition according to claim 1 or 2, wherein the weight average molecular weight (Mw) of component (A) is 10,000 or less. A resin composition comprising (A) a polycarbonate resin, (B) an epoxy resin, and (C) an inorganic filler,
The component (A) is represented by the formula (A1):
[In the formula,
Ring A and ring B each independently represent an aromatic ring which may have a substituent;
Ring X represents a non-aromatic carbocyclic ring having 7 or more carbon atoms which may have a substituent.
The polycarbonate resin contains a repeating structural unit represented by
The weight average molecular weight of the component (A) is 3,000 or more,
The hydroxyl group content of component (A) is 0.05 mmol/g or less,
The content of the component (A) is 10% by mass or more and 30% by mass or less, when the total amount of non-volatile components in the resin composition is 100% by mass,
The content of the (B) component is 3% by mass or more and 20% by mass or less, when the total amount of non-volatile components in the resin composition is 100% by mass,
The content of the component (C) is 50% by mass or more and 80% by mass or less, when the total amount of non-volatile components in the resin composition is 100% by mass,
the total content of the (A) component, the (B) component, and the (C) component is 73% by mass or more and 98% by mass or less,
the mass ratio of the polycarbonate resin (A) to the inorganic filler (C) (component (A)/component (C)) is 0.1 or more and 0.5 or less;
the dielectric loss tangent (Df) of a cured product of the resin composition is 0.0040 or less when measured at 5.8 GHz and 23°C;
A resin composition, wherein the relative dielectric constant (Dk) of a cured product of the resin composition is 3.1 or less when measured at 5.8 GHz and 23°C. The resin composition according to any one of claims 1 to 4 , wherein the component (C) is silica. The resin composition according to any one of claims 1 to 5 , further comprising (D) an epoxy resin curing agent. The resin composition according to claim 6 , wherein the component (D) comprises an active ester curing agent. The resin composition according to any one of claims 1 to 7 , further comprising (E) a radically polymerizable compound. A cured product of the resin composition according to any one of claims 1 to 8 . A sheet-like laminate material comprising the resin composition according to any one of claims 1 to 8 . A resin sheet comprising: a support; and a resin composition layer formed from the resin composition according to any one of claims 1 to 8 provided on the support. A printed wiring board comprising an insulating layer made of a cured product of the resin composition according to any one of claims 1 to 8 . A semiconductor device comprising the printed wiring board according to claim 12 .