KR20190022391A - Resin composition - Google Patents

Abstract

Provided is a resin composition which has a low dielectric constant, inhibits degradation of adhesiveness to a conductor layer due to a HAST test, and is capable of obtaining an insulating layer having a high glass transition temperature. The resin composition comprises: (A) an epoxy resin; (B) a carbodiimide compound; and (C) filler, wherein a component (C) comprises (C-1) fluorine-based filler and the amount of the component (C) is 30-80 mass%, relative to 100 mass% of a non-volatile component in the resin composition.

Description

Resin composition {RESIN COMPOSITION}

The present invention relates to a resin composition, a sheet-like laminated material, a circuit board and a semiconductor device.

BACKGROUND ART [0002] As a manufacturing technique of a circuit board, a manufacturing method by a build-up method in which an insulating layer and a conductor layer are alternately stacked on an inner layer substrate is known. The insulating layer is generally formed by obtaining a resin composition layer as a coating film of a resin varnish containing a resin composition and curing the resin composition layer. For example, Patent Document 1 discloses a resin composition comprising an epoxy resin, a curing agent and a fluorine resin filler, wherein the content of the fluorine resin filler is 50 mass% to 85 mass% with respect to the solid content of the resin composition And the resin composition is characterized.

Japanese Patent Application Laid-Open No. 2016-166347

The resin composition for forming the insulating layer generally contains a large amount of thermosetting resin from the viewpoint of achieving high insulation performance. As such a thermosetting resin, an epoxy resin and its curing agent were generally used. It is also known to use an inorganic filler as a filler to lower the thermal expansion rate of the cured product of the resin composition. On the other hand, the present inventors have studied using a fluorine-based filler as a filler in order to develop an insulating layer having a low dielectric constant.

However, the insulating layer formed by the cured product of the resin composition containing the fluorine-based filler tends to be deteriorated by the super-accelerated high-temperature high-humidity life test (HAST test) to the conductive layer formed on the insulating layer. In order to increase the insulation reliability over a long period of time, it is desired to suppress the deterioration of the adhesiveness by the HAST test.

From the viewpoint of improving the heat resistance of the insulating layer, a material for forming the insulating layer is required to have a high glass transition temperature. However, it has been difficult to increase the glass transition temperature of the cured product of the resin composition containing the fluorine-based filler.

SUMMARY OF THE INVENTION The present invention has been made in view of the above problems, and it is an object of the present invention to provide a resin composition capable of suppressing deterioration of adhesiveness to a conductor layer due to HAST test and having a low dielectric constant, A sheet-like laminate material comprising the resin composition; And a circuit board and a semiconductor device including an insulating layer made of a cured product of the resin composition.

The inventors of the present invention have made intensive studies to solve the above problems and found that by combining a predetermined amount of (C) filler containing an epoxy resin, (B) a carbodiimide compound, and (C-1) And found that the above problems can be solved, thereby completing the present invention.

That is, the present invention includes the following.

[1] A resin composition comprising (A) an epoxy resin, (B) a carbodiimide compound, and (C) a filler,

(C) comprises (C-1) a fluorine-based filler,

Wherein the amount of the component (C) is 30% by mass to 80% by mass with respect to 100% by mass of the nonvolatile component in the resin composition.

[2] The resin composition according to [1], wherein the component (C-1) is a fluorine-based polymer particle.

[3] The resin composition according to [1] or [2], wherein the component (C-1) is a polytetrafluoroethylene particle.

[4] The resin composition according to any one of [1] to [3], wherein the amount of the component (B) is 0.5% by mass to 15% by mass based on 100% by mass of the resin component in the resin composition.

[5] The composition according to [1], wherein the component (C) comprises an inorganic filler (C-2)

The resin composition according to any one of [1] to [4], wherein the amount of the component (C-2) is 5 mass% or more and 70 mass% or less based on 100 mass% of the nonvolatile component in the resin composition.

[6] The resin composition according to any one of [1] to [5], wherein the amount of the component (C-1) is 5 mass% or more and 80 mass% or less based on 100 mass% of the nonvolatile component in the resin composition.

[7] The resin composition according to any one of [1] to [7], wherein the component (A) is selected from the group consisting of a bisphenol A epoxy resin, a biquileneol epoxy resin, a biphenylaralkyl epoxy resin, a naphthylene ether epoxy resin, a naphthalene type tetrafunctional epoxy resin and a naphthol epoxy resin The resin composition according to any one of [1] to [6], wherein the epoxy resin is at least one selected from epoxy resins.

[8] The resin composition according to any one of [1] to [7], wherein the component (C-1) has an average particle diameter of 0.05 μm or more and 10 μm or less.

[9] The resin composition according to any one of [1] to [8], which contains an active ester-based curing agent.

[10] The resin composition according to any one of [1] to [9], which is used for forming an insulating layer of a circuit board.

[11] A sheet-like laminated material comprising the resin composition according to any one of [1] to [10].

[12] A circuit board comprising an insulating layer made of a cured product of the resin composition according to any one of [1] to [10].

[13] A semiconductor device comprising a circuit board according to [12].

INDUSTRIAL APPLICABILITY According to the present invention, it is possible to provide a resin composition which is low in dielectric constant, capable of suppressing a decrease in adhesiveness to a conductor layer due to the HAST test, and capable of obtaining an insulating layer having a high glass transition temperature; A sheet-like laminate material comprising the resin composition; A circuit board and a semiconductor device including the insulating layer made of the cured product of the resin composition can be provided.

Hereinafter, the present invention will be described in detail with reference to the embodiments and examples. However, the present invention is not limited to the embodiments and examples described below, and can be arbitrarily changed without departing from the scope of the claims of the present invention and its equivalent scope.

In the following description, the amount of each component in the resin composition is a value relative to 100 mass% of the nonvolatile component in the resin composition, unless otherwise specified.

In the following description, the "resin component" of the resin composition refers to a component other than the filler (C) among the nonvolatile components contained in the resin composition.

In the following description, the term " permittivity " means a dielectric constant unless otherwise specified.

[One. Outline of resin composition]

The resin composition of the present invention comprises (A) an epoxy resin, (B) a carbodiimide compound, and (C) a filler. (C) The filler includes (C-1) a fluorine-based filler. In this resin composition, the amount of the filler (C) is in a predetermined range.

The cured product of such a resin composition can lower the dielectric constant and can increase the glass transition temperature. Further, the layer of the cured product of the resin composition can suppress the deterioration of the adhesion to the conductor layer. Therefore, by using the resin composition of the present invention, it is possible to realize an insulating layer having a low dielectric constant, suppressing a decrease in adhesiveness to a conductor layer due to the HAST test, and having a high glass transition temperature. Can be obtained.

[2. (A) epoxy resin]

Examples of the epoxy resin as the component (A) include epoxy resins such as a bicyclanol type epoxy resin, a bisphenol A type epoxy resin, a bisphenol F type epoxy resin, a bisphenol S type epoxy resin, a bisphenol AF type epoxy resin, a dicyclopentadiene type epoxy resin , Trisphenol type epoxy resin, naphthol novolak type epoxy resin, phenol novolak type epoxy resin, tert-butyl-catechol type epoxy resin, naphthalene type epoxy resin, naphthol type epoxy resin, anthracene type epoxy resin, glycidyl amine type Epoxy resins, glycidyl ester type epoxy resins, cresol novolak type epoxy resins, biphenyl type epoxy resins, linear aliphatic epoxy resins, epoxy resins having a butadiene structure, alicyclic epoxy resins, heterocyclic epoxy resins, A resin, a cyclohexane type epoxy resin, a cyclohexane dimethanol type epoxy resin, a naphthylene ether Epoxy resins, there may be mentioned trimethyl olhyeong epoxy resin, tetraphenyl ethane epoxy resin. The epoxy resin may be used singly or in combination of two or more kinds.

As the epoxy resin (A), an aromatic epoxy resin is preferable from the viewpoint of lowering the average linear thermal expansion coefficient of the insulating layer. Here, the aromatic epoxy resin means an epoxy resin whose molecule contains an aromatic skeleton. The aromatic skeleton is a chemical structure generally defined as an aromatic group, and includes not only a monocyclic structure such as a benzene ring, but also a polycyclic aromatic structure such as a naphthalene ring and an aromatic heterocyclic structure. Among them, the epoxy resin (A) is preferably a bisphenol A type epoxy resin, a beacilene type epoxy resin, a biphenyl aralkyl type epoxy resin, a naphthylene ether type epoxy resin, a naphthalene type epoxy resin A tetrafunctional epoxy resin, a tetrafunctional epoxy resin and a naphthol-type epoxy resin, and a bisphenol A-type epoxy resin, a biquilene-type epoxy resin and a naphthol-type epoxy resin are particularly preferable.

The resin composition preferably contains, as the epoxy resin (A), an epoxy resin having two or more epoxy groups in one molecule. The ratio of the epoxy resin having two or more epoxy groups in one molecule to the nonvolatile component (A) of the nonvolatile component (A) of the epoxy resin is preferably 50% by mass or more, More preferably not less than 60% by mass, particularly preferably not less than 70% by mass.

As the epoxy resin, an epoxy resin (hereinafter sometimes referred to as " liquid epoxy resin ") at a temperature of 20 캜 and an epoxy resin (sometimes referred to as a " solid epoxy resin " have. The resin composition (A) may contain only liquid epoxy resin as the epoxy resin, and may contain only solid epoxy resin, but it is preferable to include a combination of liquid epoxy resin and solid epoxy resin. (A) By using a combination of a liquid epoxy resin and a solid epoxy resin as the epoxy resin, it is possible to improve the flexibility of the resin composition layer or to improve the fracture strength of the cured product of the resin composition.

As the liquid epoxy resin, a liquid epoxy resin having two or more epoxy groups in one molecule is preferable, and an aromatic liquid epoxy resin having two or more epoxy groups in one molecule is more preferable.

Examples of the liquid epoxy resin include bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol AF type epoxy resin, naphthalene type epoxy resin, glycidyl ester type epoxy resin, glycidylamine type epoxy resin, phenol novolak type epoxy resin , An alicyclic epoxy resin having an ester skeleton, a cyclohexane-type epoxy resin, a cyclohexane dimethanol-type epoxy resin, a glycidylamine-type epoxy resin, and an epoxy resin having a butadiene structure are preferable, and a glycidylamine type epoxy resin , A bisphenol A type epoxy resin, a bisphenol F type epoxy resin, a bisphenol AF type epoxy resin and a naphthalene type epoxy resin are more preferable, and a bisphenol A type epoxy resin is particularly preferable.

Specific examples of the liquid epoxy resin include " HP4032 ", " HP4032D ", " HP4032SS " (naphthalene type epoxy resin) manufactured by DIC Corporation; "828US", "jER828US", "jER828EL", "825", "Epikote 828EL" (bisphenol A type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "JER807" and "1750" (bisphenol F type epoxy resin) manufactured by Mitsubishi Chemical Corporation; &Quot; jER152 " (phenol novolak type epoxy resin) manufactured by Mitsubishi Chemical Corporation; 630 ", " 630LSD " (glycidylamine type epoxy resin) manufactured by Mitsubishi Chemical Corporation; ZX1059 " (a mixture of a bisphenol A type epoxy resin and a bisphenol F type epoxy resin) manufactured by Shinnitetsu Sumikin Kagaku Co., Ltd.; EX-721 " (glycidyl ester type epoxy resin) manufactured by Nagase ChemteX Corporation; &Quot; Celloxide 2021P " (an alicyclic epoxy resin having an ester skeleton) manufactured by Daicel Company; &Quot; PB-3600 " (epoxy resin having a butadiene structure) manufactured by Daicel Company; ZX1658 " and " ZX1658GS " (liquid 1,4-glycidyl cyclohexane type epoxy resin) manufactured by Shinnitetsu Sumikin Kagaku Co., Ltd., and the like. These may be used singly or in combination of two or more.

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

Examples of the solid epoxy resin include epoxy resins such as bicalcylenol type epoxy resins, biphenylaralkyl type epoxy resins, naphthalene type epoxy resins, naphthalene type tetrafunctional epoxy resins, cresol novolak type epoxy resins, dicyclopentadiene type epoxy resins, A bisphenol A type epoxy resin, a bisphenol AF type epoxy resin and a tetraphenyl ethane type epoxy resin are preferable, and a biscylenol type epoxy resin, a biphenyl type epoxy resin, a biphenyl type epoxy resin, a naphthylene ether type epoxy resin, an anthracene type epoxy resin, Epoxy resin, biphenylaralkyl type epoxy resin, naphthylene ether type epoxy resin, naphthalene type tetrafunctional epoxy resin and naphthol type epoxy resin are more preferable.

Specific examples of the solid epoxy resin include " HP4032H " (naphthalene type epoxy resin) manufactured by DIC Corporation; HP-4700 ", " HP-4710 " (naphthalene type tetrafunctional epoxy resin) manufactured by DIC Corporation; "N-690" (cresol novolak type epoxy resin) manufactured by DIC Corporation; "N-695" (cresol novolak type epoxy resin) manufactured by DIC Corporation; HP-7200 " (dicyclopentadiene type epoxy resin) manufactured by DIC Corporation; EXA-7311-G4 "," EXA-7311-G4S ", and" HP6000 "(manufactured by DIC Corporation," HP-7200HH "," HP-7200H "," EXA-7311 " Naphthylene ether type epoxy resin); "EPPN-502H" (trisphenol type epoxy resin) manufactured by Nippon Kayaku Co., Ltd.; NC7000L " (naphthol novolak type epoxy resin) manufactured by Nippon Kayaku Co., Ltd.; Quot; NC3000H ", " NC3000 ", " NC3000L ", and " NC3100 " (biphenylaralkyl type epoxy resin) manufactured by Nippon Kayaku Co., Ltd.; &Quot; ESN475V " (naphthol type epoxy resin) manufactured by Shinnitetsu Sumikin Kagaku Co., Ltd.; ESN485 " (naphthol novolac type epoxy resin) manufactured by Shinnitetsu Sumikin Kagaku Co., Ltd.; YX4000H ", " YX4000 ", and " YL6121 " (biphenyl type epoxy resin) manufactured by Mitsubishi Chemical Corporation; &Quot; YX4000HK " (biquileneol type epoxy resin) manufactured by Mitsubishi Chemical Corporation; "YX8800" (anthracene type epoxy resin) manufactured by Mitsubishi Chemical Corporation; &Quot; PG-100 ", " CG-500 " (Bisphenol AF type epoxy resin) manufactured by Osaka Gas Chemical Co., Ltd.; &Quot; YL7760 " (bisphenol AF type epoxy resin) manufactured by Mitsubishi Chemical Corporation; &Quot; YL7800 " (fluorene type epoxy resin) manufactured by Mitsubishi Chemical Corporation; &Quot; jER1010 " (solid bisphenol A type epoxy resin) manufactured by Mitsubishi Chemical Corporation; Quot; jER1031S " (tetraphenyl ethane type epoxy resin) manufactured by Mitsubishi Chemical Corporation. These may be used singly or in combination of two or more.

(A) When the liquid epoxy resin and the solid epoxy resin are used in combination as the epoxy resin, the mass ratio thereof (liquid epoxy resin: solid epoxy resin) is preferably 1: 0.1 to 1:15, more preferably 1 : 0.5 to 1:10, particularly preferably 1: 1 to 1: 8. When the mass ratio of the liquid epoxy resin and the solid epoxy resin is in the above range, the desirable tackiness can be obtained when used in the form of an adhesive film. Further, when used in the form of an adhesive film, sufficient flexibility can be obtained and handling properties can be improved. Further, the breaking strength of the cured product of the resin composition can be effectively increased.

The epoxy equivalent of the epoxy resin (A) is preferably 50 to 5000, more preferably 50 to 3000, still more preferably 80 to 2000, still more preferably 110 to 1000. When the epoxy equivalent of the epoxy resin (A) is in the above range, the crosslinked density of the cured product of the resin composition becomes sufficient, and an insulating layer having a small surface roughness can be obtained. The epoxy equivalent is a mass of a resin containing one equivalent of an epoxy group and can be measured according to JIS K7236.

The weight-average molecular weight of the epoxy resin (A) is preferably 100 to 5000, more preferably 250 to 3000, and still more preferably 400 to 1500, from the viewpoint of achieving the desired effect of the present invention. The weight average molecular weight of a resin such as an epoxy resin is a weight average molecular weight in terms of polystyrene measured by a gel permeation chromatography (GPC) method.

The amount of the epoxy resin (A) in the resin composition is preferably 5% by mass or more, more preferably 5% by mass or more, and more preferably 5% by mass or more, based on 100% by mass of the nonvolatile component in the resin composition, from the viewpoint of obtaining an insulating layer showing good mechanical strength and insulation reliability Is not less than 8 mass%, particularly preferably not less than 10 mass%, preferably not more than 70 mass%, more preferably not more than 69 mass%, further preferably not more than 60 mass%, particularly preferably not more than 50 mass% to be.

[3. (B) carbodiimide compound]

The carbodiimide compound as the component (B) is a compound having at least one carbodiimide group (-N═C═N-) in one molecule. By using such a carbodiimide compound (A) in combination with the epoxy resin (A) and the filler (C), it is possible to suppress the lowering of the dielectric constant and the adhesiveness to the conductor layer due to the HAST test, A high insulating layer can be obtained. As the (B) carbodiimide compound, a compound having two or more carbodiimide groups in one molecule is preferable from the viewpoint of obtaining a desired effect of the present invention remarkably. The carbodiimide compound may be used singly or in combination of two or more.

Among them, the (B) carbodiimide compound preferably contains a structural unit represented by the following formula (1).

[Chemical Formula 1]

(Wherein X represents an alkylene group, a cycloalkylene group or an arylene group, which may have a substituent, and p represents an integer of 1 to 5. When a plurality of Xs exist, they may be the same or different Also, * indicates a binding hand.)

The number of carbon atoms of the alkylene group represented by X is preferably 1 to 20, more preferably 1 to 10, still more preferably 1 to 6, still more preferably 1 to 4, 3. The number of carbon atoms of the substituent group is not included in the number of carbon atoms. Suitable examples of the alkylene group include a methylene group, an ethylene group, a propylene group and a butylene group.

The number of carbon atoms of the cycloalkylene group represented by X is preferably 3 to 20, more preferably 3 to 12, still more preferably 3 to 6. The number of carbon atoms of the substituent group is not included in the number of carbon atoms. Suitable examples of the cycloalkylene group include a cyclopropylene group, a cyclobutylene group, a cyclopentylene group and a cyclohexylene group.

The arylene group represented by X is a group having a structure in which two hydrogen atoms on aromatic rings in the aromatic hydrocarbon are excluded. The number of carbon atoms of the arylene group is preferably 6 to 24, more preferably 6 to 18, still more preferably 6 to 14, particularly preferably 6 to 10. The number of carbon atoms of the substituent group is not included in the number of carbon atoms. Suitable examples of the arylene group include a phenylene group, a naphthylene group and an anthracenylene group.

Of the alkylene group, cycloalkylene group and arylene group, X is preferably an alkylene group or a cycloalkylene group. By using an alkylene group or a cycloalkylene group, the desired effect of the present invention can be remarkably obtained. Generally, the breaking point elongation, surface roughness and fill strength of the insulating layer can be improved.

The alkylene group, cycloalkylene group and aryl group represented by X may have a substituent. Examples of the substituent include a halogen atom, an alkyl group, an alkoxy group, a cycloalkyl group, a cycloalkyloxy group, an aryl group, an aryloxy group, an acyl group and an acyloxy group.

Examples of the halogen atom as a substituent include a fluorine atom, a chlorine atom, a bromine atom and an iodine atom.

The alkyl group and the alkoxy group as a substituent may be either linear or branched. The number of carbon atoms of the alkyl group and the alkoxy group as a substituent is preferably 1 to 20, more preferably 1 to 10, still more preferably 1 to 6, still more preferably 1 to 4, 1 to 3.

The number of carbon atoms of the cycloalkyl group and cycloalkyloxy group as a substituent is preferably 3 to 20, more preferably 3 to 12, still more preferably 3 to 6.

The aryl group as a substituent is a group having a structure in which one hydrogen atom on an aromatic ring is excluded from an aromatic hydrocarbon. The number of carbon atoms of the aryl group is preferably 6 to 24, more preferably 6 to 18, still more preferably 6 to 14, particularly preferably 6 to 10.

The number of carbon atoms of the aryloxy group as a substituent is preferably 6 to 24, more preferably 6 to 18, still more preferably 6 to 14, particularly preferably 6 to 10.

The acyl group as a substituent means a group represented by the formula (2) -C (= O) -R ¹ . In the general formula (2), R ¹ represents an alkyl group or an aryl group. The alkyl group represented by R ¹ may be either linear or branched. The number of carbon atoms of R ¹ is preferably from 1 to 20, more preferably from 1 to 10, still more preferably from 1 to 6, still more preferably from 1 to 4, still more preferably from 1 to 3 . The number of carbon atoms of the aryl group represented by R ¹ is preferably 6 to 24, more preferably 6 to 18, still more preferably 6 to 14, particularly preferably 6 to 10.

The acyloxy group as a substituent means a group represented by the formula: -OC (= O) -R < ¹ >. Here, the meaning of R ¹ is the same as the meaning of R ¹ in formula (2).

Among them, as the substituent which the alkylene group, cycloalkylene group and aryl group represented by X may have, an alkyl group, an alkoxy group and an acyloxy group are preferable, and an alkyl group is more preferable.

In the general formula (1), p represents an integer of 1 to 5. Among them, p is preferably 2 or more, preferably 4 or less, and more preferably 3 or less. When p is in the above range, the desired effect of the present invention can be obtained remarkably. Generally, the breaking point elongation, surface roughness and fill strength of the insulating layer can be improved.

When a plurality of X's in formula (1) are present, they may be the same or different. In a suitable embodiment, at least one X is an alkylene group or a cycloalkylene group, which may have a substituent.

The amount of the structural unit represented by the formula (1) is preferably 50% by mass or more, more preferably 60% by mass or more, and even more preferably 70% by mass or more, relative to 100% by mass of the whole molecule of the carbodiimide compound (B) , More preferably not less than 80 mass%, particularly preferably not less than 90 mass%. The carbodiimide compound (B) may be a structural unit substantially represented by the general formula (1) except for the terminal structure. Examples of the terminal structure of the carbodiimide compound (B) include an alkyl group, a cycloalkyl group and an aryl group, and these may have a substituent. The alkyl group, cycloalkyl group or aryl group used as the terminal structure may be the same as the alkyl group, cycloalkyl group and aryl group as the substituent which the group represented by X in the formula (1) may have. The substituent which may be contained in the group used as the terminal structure may be the same as the substituent which the group represented by X in the formula (1) may have.

From the viewpoint of suppressing generation of outgassing when the resin composition is cured, the weight average molecular weight of the carbodiimide compound (B) is preferably 500 or more, more preferably 600 or more, still more preferably 700 or more, Even more preferably 800 or more, particularly preferably 900 or more, particularly preferably 1000 or more. From the viewpoint of obtaining good compatibility, the upper limit of the weight average molecular weight of the carbodiimide compound (B) is preferably 5000 or less, more preferably 4500 or less, further preferably 4000 or less, 3500 or less, particularly preferably 3,000 or less. The weight average molecular weight of the carbodiimide compound (B) can be measured as a value in terms of polystyrene by a gel permeation chromatography (GPC) method.

The carbodiimide compound (B) may originate from its production method and may contain an isocyanate group (-N = C = O) in the molecule. (B) the amount of isocyanate group (also referred to as " NCO content ") in the carbodiimide compound, from the viewpoint of obtaining a resin composition exhibiting good storage stability and realizing an insulating layer exhibiting desired properties, Is preferably 5 mass% or less, more preferably 4 mass% or less, still more preferably 3 mass% or less, still more preferably 2 mass% or less, still more preferably 1 mass% Or less.

A commercially available product of the (B) carbodiimide compound may be used. Examples of commercially available carbodiimide compounds include Carbodite (registered trademark) V-02B, V-03, V-04K, V-07 and V-09 manufactured by Nissinbo Chemical; Starpoxol (registered trademark) P, P400, and Hikaragi 510 manufactured by Rheinkmisser.

The amount of the carbodiimide compound (B) in the resin composition is preferably 0.1% by mass or more, more preferably 0.5% by mass or more, and particularly preferably 0.7% by mass or more based on 100% by mass of the resin component in the resin composition . The amount of the carbodiimide compound (B) is not less than the lower limit of the above range, the lowering of the adhesion of the insulating layer by the HAST test can be effectively suppressed, and the glass transition temperature of the cured product of the resin composition can be effectively increased. The upper limit of the amount of the (B) carbodiimide compound is preferably 20% by mass or less from the viewpoint of achieving the desired effect of the present invention. Among them, the upper limit of the amount of the carbodiimide compound (B) is more preferably 15% by mass or less, particularly preferably 15% by mass or less, from the viewpoint of increasing the resistance to elongation of the cured product of the resin composition to increase the breaking point elongation Is not more than 10% by mass.

[4. (C) Filler]

The resin composition contains a filler as the component (C). However, the (C) filler includes at least (C-1) fluorine-based filler. Therefore, the filler (C) may contain (C-1) a fluorine-based filler, and may optionally contain any filler other than the fluorine-based filler (C-1). Therefore, the resin composition may contain only the (C-1) fluorine-based filler as the filler (C), or may include the fluorine-based filler (C-1) and any filler in combination.

The amount of the filler (C) is usually 30% by mass or more, preferably 40% by mass or more, more preferably 50% by mass or more and usually 80% by mass or less based on 100% by mass of the nonvolatile component in the resin composition, Is 75 mass% or less, and more preferably 70 mass% or less. When the amount of the filler (C) containing the fluorine-based filler (C-1) is in the above range, the dielectric constant of the cured product of the resin composition can be lowered. Normally, the insulating property of the cured product of the resin composition can be enhanced by including the filler (C) in such a range. The cured product of the resin composition can suppress the deterioration of the adhesiveness of the insulating layer by the HAST test while containing the filler (C) containing the fluorine-based filler (C-1) in such a large amount.

(C-1) fluorine-based filler will be described in detail. The term " fluorine-based " means fluorine-containing. The term " fluorine-based filler " refers to a filler containing a fluorine-containing compound as a material. The filler is usually in the form of particles. Therefore, as the fluorine-based filler (C-1), particles containing a fluorine atom-containing compound are usually used.

Examples of the material of the fluorine-based filler (C-1) include a fluorine-based polymer and a fluorine-based rubber. Of these, a fluorine-based polymer is preferable from the viewpoint of reducing the dielectric constant of the insulating layer. Therefore, fluorine-based polymer particles are preferable as the fluorine-based filler (C-1).

Examples of the fluorine-based polymer include polytetrafluoroethylene (PTFE), perfluoroalkoxyalkane (PFA), perfluoroethylene propene copolymer (FEP), ethylene / tetrafluoroethylene copolymer (ETFE) (TFE / PDD), polyvinylidene fluoride (PVDF), polychlorotrifluoroethylene (PCTFE), ethylene-chlorotrifluoroethylene copolymer (ECTFE), polyfluorinated Vinyl (PVF). These may be used singly or in combination of two or more.

Of these, polytetrafluoroethylene is preferable as the fluorine-based polymer from the viewpoint of particularly reducing the dielectric constant of the insulating layer. Therefore, as the fluorine-based filler (C-1), polytetrafluoroethylene particles as particles containing polytetrafluoroethylene are preferable.

The weight average molecular weight of the fluorine-based polymer is preferably 5,000,000 or less, more preferably 4,000,000 or less, and particularly preferably 3,000,000 or less, from the viewpoint of achieving the desired effect of the present invention.

The average particle diameter of the fluorine-based filler (C-1) is preferably 0.05 μm or more, more preferably 0.08 μm or more, particularly preferably 0.10 μm or more, preferably 10 μm or less, Or less, particularly preferably 4 m or less. When the average particle diameter of the fluorine-based filler (C-1) is in the above range, the desired effect of the present invention can be obtained remarkably, and the dispersibility of the fluorine-containing filler (C-1) can do.

The average particle diameter of particles such as (C-1) fluorine-based filler can be measured by a laser diffraction / scattering method based on the Mie scattering theory. Specifically, the particle size distribution of the particles can be measured on the basis of volume by a laser diffraction scattering particle size distribution measuring apparatus, and the average particle diameter as the median diameter can be obtained from the particle size distribution thereof. The sample to be measured can be preferably those obtained by dispersing particles in a solvent such as water by ultrasonic waves. As the laser diffraction scattering type particle diameter distribution measuring apparatus, "LA-500" manufactured by Horiba Seisakusho Co., Ltd. and the like can be used.

Examples of commercially available products of the fluorine-based filler (C-1) include "Lebron L-2", "Lebron L-5", "Lebron L-5F" "FluonPTFE L-170JE", "FluonPTFEL-172JE" and "FluonPTFE L-173JE" manufactured by Asahi Glass Co., Ltd.; "KTL-500F", "KTL-2N" and "KTL-1N" manufactured by Kitamura Co., Ltd.; And " TLP10F-1 " manufactured by Mitsui-DuPont Fluorochemicals.

The fluorine-based filler (C-1) may be surface-treated. For example, the fluorine-based filler (C-1) may be surface-treated with any surface-treating agent. Examples of the surface treatment agent include surfactants such as nonionic surfactants, amphoteric surfactants, cationic surfactants and anionic surfactants; Inorganic fine particles, and the like. From the viewpoint of affinity, a fluorine-based surfactant is preferable as the surface treatment agent. As the fluorine-based surfactant, a suitable non-particulate fluorine-based polymer may be used. Specific examples of the fluorine-based surfactant include "Surflon S-243" (perfluoroalkylethylene oxide adduct) manufactured by AGC Seiyam Chemical Co., Ltd.; Megapak F-251 "," Megapack F-477 "," Megapack F-553 "," Megapark R-40 "," Megapark R-43 " "; Quot; FTX-218 ", " Futazento 610FM ", and " Futazento 730LM " manufactured by Neos.

The amount of the fluorine-based filler (C-1) in the resin composition is preferably not less than 5% by mass, more preferably not less than 10% by mass, particularly preferably not less than 20% by mass, based on 100% by mass of the non- , Preferably not more than 80 mass%, more preferably not more than 50 mass%, particularly preferably not more than 40 mass%. When the amount of the fluorine-based filler (C-1) is within the above range, the desired effect of the present invention can be obtained remarkably, and the dielectric constant of the cured product of the resin composition can be effectively reduced.

The amount of the fluorine-based filler (C-1) in the resin composition is preferably 20% by mass or more, more preferably 30% by mass or more, particularly preferably 35% by mass or more based on 100% %, Preferably not more than 100 mass%, more preferably not more than 70 mass%, particularly preferably not more than 50 mass%. When the amount of the fluorine-based filler (C-1) is within the above range, the desired effect of the present invention can be obtained remarkably, and the dielectric constant of the cured product of the resin composition can be effectively reduced.

When the resin composition contains an optional filler in combination with the (C-1) fluorine-based filler, the optional filler is preferably (C-2) an inorganic filler. By using the inorganic filler (C-2), the coefficient of thermal expansion of the cured product of the resin composition can be lowered, so that warping of the insulating layer can be effectively suppressed.

Examples of the material of the inorganic filler (C-2) include inorganic fillers such as silica, alumina, glass, cordierite, silicon oxide, barium sulfate, barium carbonate, talc, clay, mica powder, zinc oxide, hydrotalcite, , 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. Of these, silica is particularly suitable from the viewpoint of obtaining a desired effect of the present invention remarkably. Examples of the silica include amorphous silica, fused silica, crystalline silica, synthetic silica, hollow silica and the like. Among them, spherical silica is preferable. (C-2) The inorganic fillers may be used singly or in combination of two or more kinds.

Usually, the inorganic filler (C-2) is contained in the resin composition in the form of particles. The average particle diameter of the inorganic filler (C-2) is preferably not less than 0.01 탆, more preferably not less than 0.05 탆, particularly preferably not less than 0.1 탆, from the viewpoint of obtaining a desired effect of the present invention remarkably Is not more than 5.0 mu m, more preferably not more than 2.0 mu m, further preferably not more than 1.0 mu m. In addition, when the average particle diameter of the inorganic filler (C-2) is in the above range, it is possible to improve the circuit embedding property of the resin composition layer or reduce the surface roughness of the insulating layer. The average particle diameter of the inorganic filler (C-2) can be measured by a laser diffraction / scattering method based on the Mie scattering theory, similarly to the average particle diameter of the (C-1) fluorine-based filler.

(C-2) a specific surface area of the inorganic filler in terms remarkably obtain the effect of the present invention is desired, preferably 1m ² / g or more, more preferably 2m ² / g or more, and particularly preferably from 3m ² / g Or more. The upper limit is not particularly limited, but is preferably 60 m ² / g or less, 50 m ² / g or less, or 40 m ² / g or less. The specific surface area can be obtained by adsorbing nitrogen gas on the sample surface using a specific surface area measuring apparatus (Macsorb HM-1210, manufactured by Mountain Tex) according to the BET method, and calculating the specific surface area using the BET multi-point method.

Examples of commercially available products of the inorganic filler (C-2) include " SP60-05 " and " SP507-05 " manufactured by Sinetettsu Semiconductor Materials Company; "YC100C", "YA050C", "YA050C-MJE" and "YA010C" manufactured by Adomatex Corporation; "UFP-30" manufactured by Denka Corporation; "Silphil NSS-3N", "Silphil NSS-4N" and "Silpil NSS-5N" manufactured by Tokuyama Corporation; "SC2500SQ", "SO-C4", "SO-C2", and "SO-C1" manufactured by Adomex Corporation.

(C-2) The inorganic filler may be surface-treated with any surface-treating agent. Examples of the surface treatment agent include coupling agents such as amino silane coupling agents, epoxy silane coupling agents, mercaptosilane coupling agents and titanate coupling agents; Alkoxysilane compounds; And organosilazane compounds. The surface treatment with these surface treatment agents can improve the moisture resistance and dispersibility of the inorganic filler (C-2).

Examples of commercial products of surface treatment agents include KBM403 (3-glycidoxypropyltrimethoxysilane) manufactured by Shin-Etsu Chemical Co., Ltd., KBM803 (3-mercaptopropyltrimethoxy Silane), KBE903 (3-aminopropyltriethoxysilane) manufactured by Shin-Etsu Chemical Co., Ltd., KBM573 (N-phenyl-3-aminopropyltrimethoxysilane) manufactured by Shin- KBM-4803 " manufactured by Shin-Etsu Chemical Co., Ltd. (manufactured by Shin-Etsu Chemical Co., Ltd.) (long-chain epoxy type Silane coupling agents). The surface treatment agent may be used singly or in combination of two or more kinds.

The degree of surface treatment by the surface treatment agent can be evaluated by the amount of carbon per unit surface area of inorganic filler (C-2). The carbon content per unit surface area of the inorganic filler (C-2) is preferably not less than 0.02 mg / m ² , more preferably not less than 0.1 mg / m ² from the viewpoint of improving the dispersibility of the inorganic filler (C-2) Particularly preferably not less than 0.2 mg / m ² . On the other hand, in the viewpoint of suppressing an increase in the melt viscosity of the resin varnish and the melt viscosity of the sheet form, the carbon amount is preferably 1mg / m ² or less, and more preferably less, particularly preferably 0.8mg / m ² Is not more than 0.5 mg / m ² .

(C-2) The amount of carbon per unit surface area of the inorganic filler is determined by cleaning the surface-treated inorganic filler (C-2) with a solvent (for example, methyl ethyl ketone (hereinafter may be abbreviated as "MEK" Specifically, a sufficient amount of MEK and inorganic filler (C-2) surface-treated with a surface treatment agent are mixed and ultrasonically cleaned at 25 DEG C for 5 minutes. Subsequently, the supernatant is removed , And the amount of carbon per unit surface area of the inorganic filler (C-2) can be measured using a carbon analyzer after drying the nonvolatile component. As the carbon analyzer, "EMIA-320V" manufactured by Horiba Seisakusho Co., Ltd. can be used .

The amount of the inorganic filler (C-2) in the resin composition is preferably 5% by mass or more, more preferably 10% by mass or more, further preferably 15% by mass or more, relative to 100% by mass of the nonvolatile component in the resin composition , Preferably 70 mass% or less, more preferably 50 mass% or less, further preferably 40 mass% or less. (C-2) Since the amount of the inorganic filler is the lower limit value or more of the above range, the thermal expansion rate of the cured product of the resin composition can be lowered, and warping of the insulating layer can be suppressed. Further, when the amount of the inorganic filler (C-2) is not more than the upper limit of the above range, the mechanical strength of the cured product of the resin composition can be improved, and in particular, the elongation resistance can be increased and the breaking point elongation can be increased.

[5. (D) Curing agent]

The resin composition may contain (D) a curing agent as an optional component in addition to the above components. The curing agent as the component (D) usually has a function of reacting with the epoxy resin (A) to cure the resin composition. Examples of the (D) curing agent include an active ester type curing agent, a phenol type curing agent, a naphthol type curing agent, a benzoxazine type curing agent, a cyanate ester type curing agent and the like. The curing agent may be used singly or in combination of two or more kinds.

As the active ester type curing agent, a compound having at least one active ester group in one molecule can be used. Among them, examples of the active ester curing agent include compounds having two or more ester groups having high reactivity, such as phenol esters, thiophenol esters, N-hydroxyamine esters, and esters of heterocyclic hydroxy compounds, . The active ester curing agent is preferably obtained by a condensation reaction of a carboxylic acid compound and / or a thiocarboxylic acid compound with a hydroxy compound and / or a thiol compound. Particularly, from the viewpoint of improving the heat resistance, active ester type curing agents obtained from carboxylic acid compounds and hydroxy compounds are preferable, and active ester type curing agents obtained from carboxylic acid compounds and phenol compounds and / or naphthol compounds are more preferable.

Examples of the carboxylic acid compound include benzoic acid, acetic acid, succinic acid, maleic acid, itaconic acid, phthalic acid, isophthalic acid, terephthalic acid and pyromellitic acid.

Examples of the phenol compound or naphthol compound include hydroquinone, resorcin, bisphenol A, bisphenol F, bisphenol S, phenolphthalein, methylated bisphenol A, methylated bisphenol F, methylated bisphenol S, phenol, o- Cresol, catechol, alpha -naphthol, beta -naphthol, 1,5-dihydroxynaphthalene, 1,6-dihydroxynaphthalene, 2,6-dihydroxynaphthalene, dihydroxybenzophenone, Trihydroxybenzophenone, tetrahydroxybenzophenone, fluoroglucine, benzene triol, dicyclopentadiene type diphenol compounds, phenol novolak, and the like. Here, the "dicyclopentadiene type diphenol compound" refers to a diphenol compound obtained by condensing two molecules of phenol in one dicyclopentadiene molecule.

Specific preferred examples of the active ester-based curing agent include active ester compounds containing a dicyclopentadiene type diphenol structure, active ester compounds containing a naphthalene structure, active ester compounds containing an acetylated phenol novolac, And an active ester compound including a benzoylate. Of these, active ester compounds containing a naphthalene structure and active ester compounds containing a dicyclopentadiene type diphenol structure are more preferable. The "dicyclopentadiene-type diphenol structure" refers to a divalent structural unit consisting of phenylene-dicyclopentylene-phenylene.

EXB9451 "," EXB9460 "," EXB9460S "," HPC-8000-65T "," HPC-8000-65T ", and" HPC-8000-65T "as active ester compounds containing a dicyclopentadiene type diphenol structure as commercial products of the active ester- -8000H-65TM, EXB-8000L-65TM and EXB-8150-65T (manufactured by DIC); EXB9416-70BK " (manufactured by DIC) as an active ester compound containing a naphthalene structure; &Quot; DC808 " (manufactured by Mitsubishi Chemical Corporation) as an active ester compound containing acetylated phenol novolak; &Quot; YLH1026 " (manufactured by Mitsubishi Chemical Corporation) as an active ester compound containing a benzoylate of phenol novolak; &Quot; DC808 " (manufactured by Mitsubishi Chemical Corporation) as an active ester-based curing agent which is acetylated phenol novolak; YLH1026 " (manufactured by Mitsubishi Chemical Corporation), " YLH1030 " (manufactured by Mitsubishi Chemical Corp.), and YLH1048 (manufactured by Mitsubishi Chemical Corporation) as the benzoylates of phenol novolak.

As the phenol-based curing agent and naphthol-based curing agent, those having a novolak structure are preferable from the viewpoints of heat resistance and water resistance. From the viewpoint of adhesion between the insulating layer and the conductor layer, a nitrogen-containing phenol-based curing agent is preferable, and a phenazine-based curing agent containing a triazine skeleton is more preferable.

Specific examples of the phenol-based curing agent and naphthol-based curing agent include "MEH-7700", "MEH-7810" and "MEH-7851" manufactured by Meiwa Kasei; NHN ", " CBN ", " GPH ", manufactured by Nippon Kayaku Co., "SN170", "SN180", "SN190", "SN475", "SN485", "SN495", "SN-495V" and "SN375" manufactured by Shinnitetsu Sumi- TD-2090 "," LA-7052 "," LA-7054 "," LA-1356 "," LA-3018-50P "and" EXB-9500 "manufactured by DIC Corporation.

Specific examples of the benzoxazine type curing agent include "HFB2006M" manufactured by Showa Kobunshi Co., Ltd., "P-d" manufactured by Shikoku Kasei Corporation, and "F-a".

Examples of the cyanate ester curing agent include bisphenol A dicyanate, polyphenol cyanate, oligo (3-methylene-1,5-phenylene cyanate), 4,4'- Dimethylphenyl cyanate), 4,4'-ethylidenediphenyl dicyanate, hexafluorobisphenol A dicyanate, 2,2-bis (4-cyanate) phenylpropane, 1,1- Cyanate phenylmethane), bis (4-cyanate-3,5-dimethylphenyl) methane, 1,3-bis Naphthyl phenyl) thioether, and bis (4-cyanate phenyl) ether; Polyfunctional cyanate resins derived from phenol novolak and cresol novolak; And prepolymerized prepolymers of these cyanate resins. Specific examples of the cyanate ester curing agent include "PT30" and "PT60" (phenol novolac type polyfunctional cyanate ester resin), "ULL-950S" (multifunctional cyanate ester resin), "BA230 BA230S75 " (a prepolymer obtained by trimerizing a part or all of bisphenol A dicyanate to form a trimer), and the like.

Among the above, as the (D) curing agent, an active ester-based curing agent is preferable. By using the active ester type curing agent, the desired effect of the present invention can be obtained remarkably. In particular, since the carbodiimide compound (B) has an effect of inhibiting the hydrolysis of the ester bond, (B) the carbodiimide compound and the active ester-based curing agent are used in combination, Deterioration can be suppressed and deterioration of the adhesion of the insulating layer to the conductor layer can be effectively suppressed. Therefore, the (D) curing agent used in the resin composition preferably contains an active ester-based curing agent.

When the active ester type curing agent is used, the amount of the active ester type curing agent relative to 100 mass% of the (D) curing agent is preferably 20 mass% or more, more preferably 30 mass% or more, still more preferably 35 mass% , Preferably 80 mass% or less, more preferably 70 mass% or less, further preferably 60 mass% or less. When the amount of the active ester curing agent is in the above range, deterioration of the adhesion of the insulating layer to the conductor layer by the HAST test can be effectively suppressed.

When the active ester-based curing agent is used, the amount of the active ester-based curing agent relative to 100 mass% of the (B) carbodiimide compound is preferably from the viewpoint of effectively suppressing the adhesiveness of the insulating layer to the conductor layer by the HAST test Is at least 5% by mass, more preferably at least 10% by mass, and even more preferably at least 15% by mass. Among them, the amount of the active ester-based curing agent is preferably 20% by mass or more, more preferably 30% by mass or more, particularly preferably 30% by mass or more, from the viewpoint of increasing the resistance to elongation of the cured product of the resin composition and increasing the breaking point elongation Is at least 50% by mass. There is no upper limit, for example, 2000 mass%.

When the (D) curing agent is used, the amount of the (D) curing agent in the resin composition is preferably 0.1% by mass or more, more preferably 0.1% by mass or more, More preferably not less than 0.5% by mass, further preferably not less than 1% by mass, preferably not more than 30% by mass, more preferably not more than 20% by mass, further preferably not more than 10% by mass.

When the number of epoxy groups in the epoxy resin (A) is 1, the number of active groups in the (D) curing agent is preferably 0.05 or more, more preferably 0.1 or more, still more preferably 0.15 or more, More preferably 1.5 or less, further preferably 1 or less, particularly preferably 0.8 or less. Here, the "epoxy group number of the epoxy resin (A)" is a value obtained by adding up the values obtained by dividing the mass of the nonvolatile component (A) of the epoxy resin present in the resin composition by the epoxy equivalent. The term "(D) the number of active groups of the curing agent" is a value obtained by adding up the values obtained by dividing the mass of the nonvolatile component of the curing agent (D) present in the resin composition by the active group equivalent. When the number of epoxy groups in the epoxy resin (A) is 1 and the number of active groups of the (D) curing agent is in the above range, the desired effect of the present invention can be obtained remarkably, and the heat resistance of the cured product .

[6. (E) Thermoplastic resin]

The resin composition may contain (E) a thermoplastic resin as an optional component in addition to the above components. Examples of the thermoplastic resin as the component (E) include thermoplastic resins such as phenoxy resin, polyvinyl acetal resin, polyolefin resin, polybutadiene resin, polyimide resin, polyamideimide resin, polyetherimide resin, polysulfone resin, Resins, polyphenylene ether resins, polycarbonate resins, polyether ether ketone resins, and polyester resins. Among them, a phenoxy resin is preferable from the viewpoint of obtaining a desired effect of the present invention remarkably. The thermoplastic resin may be used singly or in combination of two or more kinds.

Examples of the phenoxy resin include bisphenol A skeleton, bisphenol F skeleton, bisphenol S skeleton, bisphenol acetophenone skeleton, novolac skeleton, biphenyl skeleton, fluorene skeleton, dicyclopentadiene skeleton, norbornene skeleton, naphthalene skeleton, A phenoxy resin having at least one skeleton selected from the group consisting of a skeleton, an anthracene skeleton, an adamantane skeleton, a terpene skeleton, and a trimethyl cyclohexane skeleton. The terminal of the phenoxy resin may be any functional group such as a phenolic hydroxyl group or an epoxy group.

Specific examples of the phenoxy resin include " 1256 " and " 4250 " (phenoxy resin containing bisphenol A skeleton) manufactured by Mitsubishi Chemical Corporation; &Quot; YX8100 " (bisphenol S skeleton-containing phenoxy resin) manufactured by Mitsubishi Chemical Corporation; "YX6954" (a phenoxy resin containing a bisphenol acetophenone skeleton) manufactured by Mitsubishi Chemical Corporation; &Quot; FX280 " and " FX293 " manufactured by Shinnitetsu Sumikin Kagaku; YL6954BH30, YL7769BH30, YL6794, YL7213, YL7290, YL7891BH30, and YL7482 manufactured by Mitsubishi Chemical Corporation.

The weight average molecular weight of the thermoplastic resin (E) in terms of polystyrene is preferably 8000 or more, more preferably 10000 or more, particularly preferably 20000 or more, and preferably 70000 or more, in view of obtaining a desired effect of the present invention remarkably. More preferably not more than 60000, particularly preferably not more than 50000. The weight average molecular weight of the thermoplastic resin (E) in terms of polystyrene can be measured by a gel permeation chromatography (GPC) method.

When the thermoplastic resin (E) is used, the amount of the thermoplastic resin (E) in the resin composition is preferably 0.5% by mass or more, more preferably 0.6% by mass or more, Preferably 0.7 mass% or more, preferably 15 mass% or less, more preferably 12 mass% or less, further preferably 10 mass% or less.

[7. (F) Curing accelerator]

In addition to the above-mentioned components, the resin composition may further contain (C) a curing accelerator as an optional component. By using the (F) curing accelerator, curing can be promoted when the resin composition is cured.

Examples of the curing accelerator (F) include phosphorus hardening accelerators, amine hardening accelerators, imidazole hardening accelerators, guanidine hardening accelerators, metal hardening accelerators and peroxide hardening accelerators. Among them, phosphorus hardening accelerator, amine hardening accelerator, imidazole hardening accelerator and metal hardening accelerator are preferable, and amine hardening accelerator, imidazole hardening accelerator and metal hardening accelerator are more preferable, and amine hardening accelerator is particularly preferable desirable. The curing accelerator (F) may be used singly or in combination of two or more kinds.

Examples of phosphorus hardening accelerators include triphenylphosphine, phosphonium borate compounds, tetraphenylphosphonium tetraphenylborate, n-butylphosphonium tetraphenylborate, tetrabutylphosphonium decanoate, (4-methylphenyl) triphenyl Phosphonium thiocyanate, tetraphenylphosphonium thiocyanate, and butyltriphenylphosphonium thiocyanate. Among them, triphenylphosphine and tetrabutylphosphonium decanoate are preferable.

Examples of the amine-based curing accelerator include trialkylamines such as triethylamine and tributylamine, 4-dimethylaminopyridine, benzyldimethylamine, 2,4,6-tris (dimethylaminomethyl) - diazabicyclo (5,4,0) undecene. Among them, 4-dimethylaminopyridine and 1,8-diazabicyclo (5,4,0) -undecene are preferable.

Examples of the imidazole-based curing accelerator include 2-methylimidazole, 2-undecylimidazole, 2-heptadecylimidazole, 1,2-dimethylimidazole, Imidazole, 1,2-dimethylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2-phenyl- Benzyl-2-phenylimidazole, 1-cyanoethyl-2-methylimidazole, 1-cyanoethyl-2-undecylimidazole, 1-cyanoethyl- 1-cyanoethyl-2-phenylimidazole, 1-cyanoethyl-2-undecylimidazolium trimellitate, 1-cyanoethyl-2-phenylimidazolium Trimellitate, 2,4-diamino-6- [2'-methylimidazolyl- (1 ')] -ethyl-s-triazine, 2,4- diamino-6- [ Imidazolyl- (1 ')] - ethyl-s-triazine, 2,4-diamino-6- [2'-ethyl-4'-methylimidazolyl- Triazine, 2,4-diamino-6- [2'-methylimidazolyl- (1 ')] - ethyl- , 2-phenylimidazole isocyanuric acid adduct, 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 Imidazole compounds; And adducts of an imidazole compound and an epoxy resin. Among them, 2-ethyl-4-methylimidazole and 1-benzyl-2-phenylimidazole are preferable.

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

Examples of the guanidine curing accelerator include dicyandiamide, 1-methylguanidine, 1-ethylguanidine, 1-cyclohexylguanidine, 1-phenylguanidine, 1- (o-tolyl) guanidine, dimethylguanidine, , Trimethylguanidine, tetramethylguanidine, pentamethylguanidine, 1,5,7-triazabicyclo [4.4.0] deca-5-ene, 7-methyl-1,5,7-triazabicyclo [4.4.0] 1-n-butylbiguanide, 1-n-octadecylbiguanide, 1,1-dimethylbiguanide, 1, 1-cyclohexylbiguanide, 1-allylbiguanide, 1-phenylbiguanide, and 1- (o-tolyl) biguanide. Among them, dicyandiamide, 1,5,7-triazabicyclo [4.4.0] deca-5-ene is preferable.

Examples of the metal-based curing accelerator include organic metal complexes or organic metal salts of metals such as cobalt, copper, zinc, iron, nickel, manganese and tin. Specific examples of the organometallic complexes include organic cobalt complexes such as cobalt (II) acetylacetonate and cobalt (III) acetylacetonate, organic copper complexes such as copper (II) acetylacetonate, zinc An organic iron complex such as an organic zinc complex and iron (III) acetylacetonate, an organic nickel complex such as nickel (II) acetylacetonate, and an organic manganese complex such as manganese (II) acetylacetonate. Examples of the organic metal salt include zinc octylate, tin octylate, zinc naphthenate, cobalt naphthenate, tin stearate, and zinc stearate.

Examples of the peroxide-based curing accelerator include cyclohexanone peroxide, tert-butylperoxy benzoate, methyl ethyl ketone peroxide, dicumyl peroxide, tert-butyl cumyl peroxide, di- Propylbenzene hydroperoxide, cumene hydroperoxide, and tert-butyl hydroperoxide.

As the peroxide-based curing accelerator, a commercially available product can be used, and for example, " PERCUMIL D "

When the (F) curing accelerator is used, the amount of the (C) curing accelerator in the resin composition is preferably 0.01 mass% or more, more preferably 0.01 mass% or less, , More preferably not less than 0.03 mass%, particularly preferably not less than 0.05 mass%, preferably not more than 3 mass%, more preferably not more than 2 mass%, particularly preferably not more than 1 mass%.

[8. (G) fluoropolymer or fluoric oligomer]

The resin composition may contain a non-particulate (G) fluoropolymer or fluoric oligomer as an optional component in addition to the above components. As the fluorine-based polymer and the fluorine-based oligomer as the component (G), only the fluorine-based polymer may be used, only the fluorine-based oligomer may be used, and the fluorine-based polymer and the fluorine-based oligomer may be used in combination. The component (G) is a component that can be a non-particulate phase in the resin composition and is usually excellent in compatibility with a resin component such as (A) an epoxy resin. Further, the component (G) contains a fluorine atom in its molecule, and thus has a high affinity for the (C-1) fluorine-based filler. Therefore, the component (G) functions as a surfactant at the interface between the fluorine-containing filler (C-1) and the resin component, and can improve the dispersibility of the fluorine-containing filler (C-1). Further, the surface roughness of the insulating layer after the roughening treatment can be reduced by increasing the dispersibility of the fluorine-based filler (C-1). By using the component (G), the dielectric constant of the cured product of the resin composition can be generally lowered.

As the fluorine-based polymer, for example, "LE-605" manufactured by Kyowa Chemical Co., Ltd. and the like can be mentioned. Examples of the fluorinated oligomers include Megapak® F-556, F-558, F-561, F-563, F-569, DS- R-40 ", " R-41 ", and the like. The component (G) may be used singly or in combination of two or more.

When the component (G) is used, the amount of the component (G) in the resin composition is preferably 0.1% by mass or more, more preferably 0.5% by mass or more, particularly preferably 100% Is not less than 1.0% by mass, preferably not more than 10% by mass, more preferably not more than 5% by mass, particularly preferably not more than 3% by mass. When the amount of the component (G) is in the above range, the surface roughness of the insulating layer after the roughening treatment can be reduced or the dielectric constant of the cured product of the resin composition can be effectively lowered.

[9. (H) coupling agent]

The resin composition may contain (H) a coupling agent as an optional component in addition to the above components. (H) coupling agent can be used to increase the dispersibility of the inorganic filler (C-2), so that the surface roughness of the insulating layer after the roughening treatment can be reduced.

As the (H) coupling agent, there may be mentioned, for example, (C-2) the examples of the surface treatment agent of the inorganic filler. The coupling agent (H) may be used singly or in combination of two or more kinds.

(H) coupling agent is used, the amount of the (H) coupling agent in the resin composition is preferably 0.1% by mass or more, more preferably 0.2% by mass or more, Preferably 0.5% by mass or more, preferably 5% by mass or less, more preferably 3% by mass or less, and particularly preferably 1% by mass or less. When the amount of the (H) coupling agent is in the above range, the surface roughness of the insulating layer after the roughening treatment can be reduced.

[10. (I) Additive]

In addition to the above-mentioned components, the resin composition may further contain additives as optional components. Examples of such additives include organic metal compounds such as organic copper compounds, organic zinc compounds and organic cobalt compounds; Thickener; Defoamer; Leveling agents; An adhesion imparting agent; coloring agent; Flame retardants and the like. The additives may be used singly or in combination of two or more.

[11. Method of producing resin composition]

The resin composition can be produced, for example, by mixing a compounding component with a solvent as required and stirring by using a stirring device such as a rotary mixer. Particularly, when the component (G) is used, the fluorine-containing filler (C) is mixed with the fluorine-containing filler and the component (G) Mixing is preferred. Thereby, the dispersibility of the fluorine-based filler (C-1) can be increased, and the surface roughness of the insulating layer after the roughening treatment can be reduced.

[12. Characteristics of Resin Composition]

The cured product of the above resin composition can lower its dielectric constant. Therefore, an insulating layer having a low dielectric constant can be obtained by the cured product of the resin composition. For example, when a cured product is obtained by curing the resin composition by the method described in the examples, the dielectric constant of the cured product is preferably 3.00 or less, more preferably 2.90 or less, particularly preferably 2.80 or less have. Here, the dielectric constant of the cured product can be measured by the method described in the embodiment.

The cured product of the above resin composition can increase its glass transition temperature. Therefore, an insulating layer having excellent heat resistance can be obtained by the cured product of the resin composition. For example, when a cured product is obtained by curing the resin composition by the method described in the examples, the glass transition temperature of the cured product is preferably 145 ° C or more, more preferably 150 ° C or more, particularly preferably 160 Lt; 0 > C or more. Here, the glass transition temperature of the cured product can be measured by the method described in the Examples.

When the conductive layer is formed on the layer of the cured product of the resin composition described above, it is possible to suppress deterioration of the adhesion between the layer of the cured product and the conductive layer. More specifically, it is possible to suppress deterioration of the adhesion in a high temperature and high humidity environment. Therefore, with the cured product of the resin composition described above, it is possible to obtain an insulating layer capable of suppressing the deterioration of the adhesion to the conductor layer by the HAST test. For example, in the case where the insulating layer is formed by the cured product of the resin composition and the conductor layer is formed by plating on the insulating layer by the method described in the embodiment, the fill of the HAST test under the conditions described in the embodiment The rate of decrease in the strength can be set within a predetermined range. Concretely, the rate of decrease in the peel strength is preferably 50% or less, more preferably 40% or less, particularly preferably 30% or less. The rate of decrease of the peel strength can be measured by the method described in Examples.

When the conductive layer is formed on the layer of the cured product of the resin composition, the adhesion between the layer of the cured product and the conductive layer can be generally increased. Therefore, according to the cured product of the resin composition described above, an insulating layer having high adhesion to a conductor layer can be obtained. For example, when the insulating layer is formed by the cured product of the resin composition and the conductor layer is formed on the insulating layer by plating in the method described in the embodiment, the peel strength can be increased. Specifically, the fill strength may preferably be 0.2 kgf / cm or more, more preferably 0.3 kgf / cm or more, and particularly preferably 0.4 kgf / cm or more. The peel strength can be measured by the method described in the Examples.

The cured product of the resin composition usually has excellent resistance to elongation, so that even if it is stretched, it is hard to cause breakage. Therefore, according to the cured product of the resin composition described above, an insulating layer having an excellent mechanical strength can be obtained. For example, when the cured resin film is obtained by curing the resin composition by the method described in the embodiment, the elongation at break of the cured film is preferably 0.5% or more, more preferably 0.7% or more, particularly preferably 0.7% Can be 0.9% or more. The breaking point elongation can be measured by the method described in the examples.

The surface roughness of the cured product of the resin composition after the roughening treatment can be reduced in general when the roughening treatment is carried out. Therefore, according to the above-mentioned cured product of the resin composition, an insulating layer having a small surface roughness can be obtained. For example, when the insulating layer is formed by the cured product of the resin composition and the insulating layer is roughened by the method described in the embodiment, the surface roughness of the insulating layer after the roughening treatment can be made to fall within a predetermined range have. Specifically, the surface roughness is an arithmetic mean roughness (Ra), preferably 300 nm or less, more preferably 280 nm or less, particularly preferably 250 nm or less. The surface roughness is a 10-point average roughness (Rz), preferably 5.0 탆 or less, more preferably 4.5 탆 or less, and particularly preferably 4.0 탆 or less.

[13. Use of Resin Composition]

The resin composition of the present invention can be used as a resin composition for forming an insulating layer of a circuit board such as a printed circuit board. The insulating layer includes an insulating layer for forming a conductor layer (including a rewiring layer) on the insulating layer. Therefore, the resin composition may be used as a resin composition for forming an insulating layer for forming a conductor layer. Among them, the resin composition is preferably used as a resin composition for forming a build-up insulating layer for forming an insulating layer in the production of a circuit board by a build-up method.

In particular, taking advantage of the fact that an insulating layer with a low dielectric constant can be obtained, the resin composition is preferably used as a resin composition (resin composition for forming an insulating layer of a high-frequency circuit substrate) for forming an insulating layer of a high- . Among them, the resin composition can be more suitably used as a resin composition (a resin composition for forming an interlayer insulating layer of a high-frequency circuit substrate) for forming an interlayer insulating layer of a high-frequency circuit board. Here, the " high frequency circuit board " means a circuit board capable of operating even an electric signal of a high frequency band. The term " high-frequency band " means a band of 1 GHz or higher, and the resin composition is particularly effective in a band of 28 GHz to 80 GHz.

In addition, the insulating layer having a low dielectric constant contributes to lowering the height of the circuit board, which is suitable for applications requiring a thin circuit board. Further, the insulating layer having a low dielectric constant facilitates impedance control of the circuit board, which is suitable for increasing the degree of design freedom of the circuit board. From such a viewpoint, a suitable use of the resin composition is, for example, a circuit board such as a mother board, an IC package substrate, a camera module substrate, or a substrate for a fingerprint authentication sensor used in a portable device. Specifically, for example, the fingerprint authentication sensor may include an insulating layer included in a circuit board, a plurality of electrodes formed on the insulating layer, and an insulating coating in this order. In this fingerprint authentication sensor, the authentication of the fingerprint is carried out by using a capacitance value formed by the finger, the electrode, and the insulating film on the insulating film different from the concave portion and the convex portion of the fingerprint. In such a fingerprint authentication sensor, if the insulating layer can be made thinner, the size of the sensor itself can be reduced.

In addition, the resin composition of the present invention can be used for a wide range of applications in which a resin composition such as a sheet-like laminate material such as an adhesive film or a prepreg, a solder resist, an underfill material, a die bonding material, a semiconductor sealing material, Can be used.

[14. Sheet laminated material]

The resin composition described above can be applied in a varnish state to form an insulating layer. However, it is industrially preferable to use it in the form of a sheet-like laminate material containing the resin composition. Preferable examples of the sheet-like laminated material include an adhesive film and a prepreg.

In one embodiment, the adhesive film comprises a support and a resin composition layer provided on the support. The resin composition layer is a layer formed of the resin composition described above and may be referred to as an " adhesive layer ".

The thickness of the resin composition layer is preferably 100 占 퐉 or less, more preferably 80 占 퐉 or less, still more preferably 60 占 퐉 or less, and most preferably 50 占 퐉 or less, from the viewpoint of thinning. The lower limit of the thickness of the resin composition layer is not particularly limited and may be, for example, 1 占 퐉 or more, 5 占 퐉 or more, 10 占 퐉 or more and the like.

As the support, for example, a film made of a plastic material, a metal foil, and a release paper can be given. As the support, a film or a metal foil made of a plastic material is preferable.

When a film made of a plastic material is used as the support, examples of the plastic material include polyethylene terephthalate (hereinafter may be referred to as "PET"), polyethylene naphthalate (hereinafter sometimes referred to as "PEN" Polyester; Polycarbonate (hereinafter sometimes referred to as " PC "); Acrylic polymers such as polymethyl methacrylate (hereinafter sometimes referred to as " PMMA "); Cyclic polyolefin; Triacetylcellulose (hereinafter sometimes referred to as " TAC "); Polyether sulfide (hereinafter sometimes referred to as " PES "); Polyether ketones; Polyimide. Of these, polyethylene terephthalate and polyethylene naphthalate are preferable, and polyethylene terephthalate is particularly preferable since it is inexpensive and excellent in availability.

When a metal foil is used as a support, examples of the metal foil include copper foil and aluminum foil. Among them, a copper foil is preferable. As the copper foil, a foil made of a copper metal may be used, or a foil made of an alloy of copper and another metal (for example, tin, chromium, silver, magnesium, nickel, zirconium, silicon, It is also good.

The support may be subjected to a treatment such as a mat treatment, a corona treatment, and an antistatic treatment on the surface to be bonded to the resin composition layer.

As the support, a support having a release layer having a release layer on the surface to be bonded to the resin composition layer may be used. Examples of the release agent that can be used for the release layer of the release layer-adhered support include one or more types of release agents selected from the group consisting of an alkyd resin, a polyolefin resin, a urethane resin, and a silicone resin. Examples of commercially available products of the release agent include "SK-1", "AL-5", and "AL-7" manufactured by Lin Tec Corporation, which is an alkyd resin type release agent. As the release layer-adhered support, for example, " Lumirror T60 " "Purex" manufactured by Dejin Corporation; And " Unipyl " manufactured by Uni-Chika Corporation.

The thickness of the support is preferably in the range of 5 탆 to 75 탆, more preferably in the range of 10 탆 to 60 탆. When the release layer-adhered support is used, it is preferable that the thickness of the entirety of the release layer-adhered support is in the above range.

The adhesive film can be formed, for example, by preparing a resin varnish containing an organic solvent and a resin composition, applying the resin varnish to a support using a coating device such as a die coater, and drying the resin varnish to form a resin composition layer Can be manufactured.

Examples of the organic solvent include ketone solvents such as acetone, methyl ethyl ketone (MEK) and cyclohexanone; Acetic acid ester solvents such as ethyl acetate, butyl acetate, cellosolve acetate, propylene glycol monomethyl ether acetate and carbitol acetate; Carbitol solvents such as cellosolve and butyl carbitol; Aromatic hydrocarbon solvents such as toluene and xylene; And amide solvents such as dimethylformamide, dimethylacetamide (DMAc) and N-methylpyrrolidone. The organic solvents may be used alone or in combination of two or more.

The drying can be carried out by a known method such as heating or hot air spraying. The drying conditions are set so that the content of the organic solvent in the resin composition layer is usually 10 mass% or less, preferably 5 mass% or less. For example, 30 to 60% by mass, is used, the resin varnish is dried at 50 to 150 캜 for 3 minutes to 10 minutes, whereby the resin composition Layer can be formed. Usually, the resin composition layer is obtained as a film obtained by half-curing the coating film of the resin varnish.

The adhesive film may optionally include a layer other than the support and the resin composition layer. For example, a protective film according to a support may be provided on the surface of the adhesive film which is not bonded to the support of the resin composition layer (that is, the surface opposite to the support). The thickness of the protective film is, for example, 1 占 퐉 to 40 占 퐉. By the protective film, adhesion and scratches of dust or the like to the surface of the resin composition layer can be suppressed. When the adhesive film has a protective film, the adhesive film is usually usable by peeling the protective film. Further, the adhesive film can be rolled and stored.

In one embodiment, the prepreg can be formed by impregnating a sheet-like fibrous substrate with a resin composition.

The sheet-like fibrous substrate used in the prepreg is not particularly limited. As the sheet-like fiber base material, any fiber base material used as a base material for a prepreg such as glass cloth, aramid nonwoven fabric, liquid crystal polymer nonwoven fabric and the like can be used. From the viewpoint of thinning, the thickness of the sheet-like fiber base material is preferably 900 占 퐉 or less, more preferably 800 占 퐉 or less, further preferably 700 占 퐉 or less, particularly preferably 600 占 퐉 or less. The thickness of the sheet-like fiber base material is preferably 30 占 퐉 or less, more preferably 20 占 퐉 or less, and particularly preferably 10 占 퐉 or less, from the viewpoint of suppressing the locking depth of the plating in forming the conductor layer. The lower limit of the thickness of the sheet-like fiber base material is usually 1 占 퐉 or more, 1.5 占 퐉 or more, or 2 占 퐉 or more.

The prepreg can be produced by a method such as a hot melt method or a solvent method. The thickness of the prepreg may be the same as that of the resin composition layer in the adhesive film.

[15. Circuit board]

The circuit board of the present invention includes an insulating layer formed of a cured product of the above resin composition. In one embodiment, the circuit board includes an inner layer substrate and an insulating layer provided on the inner layer substrate.

The " inner layer substrate " is a member serving as a substrate of a circuit substrate. Examples of the inner-layer substrate include a core substrate such as a glass epoxy substrate, a metal substrate, a polyester substrate, a polyimide substrate, a BT resin substrate, and a thermosetting polyphenylene ether substrate. Further, usually, the inner layer substrate has a conductor layer formed directly or indirectly on one or both surfaces of the core substrate. The conductor layer may be patterned to function as, for example, an electric circuit. An inner layer substrate on which a conductor layer is formed as a circuit on one side or both sides of the core substrate is sometimes referred to as an " inner layer circuit substrate ". Further, an intermediate product to which at least one of the insulating layer and the conductor layer is to be additionally formed for manufacturing the circuit board is also included in the term " inner layer substrate ". In the case where the circuit board incorporates a component, an inner-layer board containing components may be used.

The thickness of the inner layer substrate is usually from 50 mu m to 4000 mu m and preferably from 200 mu m to 3200 mu m from the standpoint of improvement of the mechanical strength of the circuit board and reduction in thickness (reduction in thickness).

The inner layer substrate may be provided with one or more through holes extending from one surface to the other surface in order to electrically connect the conductor layers on both sides thereof. Further, the inner-layer substrate may have additional components such as passive elements.

The insulating layer is a layer of a cured product of the resin composition. The insulating layer formed of the cured product is particularly suitable for circuit boards such as motherboards, IC package substrates, camera module substrates, and fingerprint authentication sensor substrates used for circuit boards, high frequency circuit boards, and portable devices by build- The present invention can be suitably applied to an insulating layer.

The circuit board may have only one insulating layer or two or more insulating layers. When the circuit board has an insulating layer having two or more layers, it can be provided as a build-up layer in which a conductor layer and an insulating layer are alternately stacked.

The thickness of the insulating layer is usually 20 占 퐉 to 200 占 퐉, preferably 50 占 퐉 to 150 占 퐉, from the viewpoints of improvement of electrical characteristics and lowering of the circuit board.

The insulating layer may be provided with one or more via holes for electrically connecting the conductor layers of the circuit board to each other.

Since the insulating layer is a layer formed by the cured product of the resin composition described above, the cured product of the resin composition can exert excellent properties. Therefore, the insulating layer of the circuit board preferably has a dielectric constant of the insulating layer, a glass transition temperature, a reduction ratio by the HAST test of the fill strength between the insulating layer and the conductive layer, a peel strength between the insulating layer and the conductive layer, , The surface roughness after the roughening treatment can be adjusted to the range as described in the section of the properties of the resin composition. These properties can also be measured by the methods described in the examples.

The circuit board can be manufactured by a manufacturing method including the following steps (I) and (II) using, for example, an adhesive film.

(I) A step of laminating an adhesive film on the inner layer substrate and a resin composition layer of the adhesive film bonded to the inner layer substrate.

(II) A step of thermally curing the resin composition layer to form an insulating layer.

The lamination of the inner layer substrate and the adhesive film can be performed, for example, by a heat pressing process in which the adhesive film is heated while being pressed against the inner layer substrate from the support side. Examples of members (also referred to as " hot pressing members ") for a hot pressing process include a heated metal plate (SUS hard plate) or a metal roll (SUS roll). Further, it is preferable to press the hot pressing member through an elastic material such as heat-resistant rubber so that the adhesive film sufficiently follows the unevenness of the surface of the inner layer substrate, rather than directly pressing the hot pressing member against the support of the adhesive film.

The lamination of the inner layer substrate and the adhesive film can be carried out, for example, by a vacuum laminating method. The temperature of the hot pressing in the vacuum laminating method is preferably 60 ° C to 160 ° C, more preferably 80 ° C to 140 ° C. The pressure of the hot pressing is preferably 0.098 MPa to 1.77 MPa, more preferably 0.29 MPa to 1.47 MPa. The time for hot pressing is preferably 20 seconds to 400 seconds, more preferably 30 seconds to 300 seconds. The lamination is preferably performed under a reduced pressure of 26.7 hPa or less.

The lamination can be performed by a commercially available vacuum laminator. As a commercially available vacuum laminator, for example, a vacuum pressurized laminator manufactured by Meikisai Sakusho Co., Ltd., a vacuum applicator manufactured by Nikko Material Co., Ltd., a vacuum type vacuum laminator, and the like can be given.

After lamination, the laminated resin composition layer may be subjected to a smoothing treatment under atmospheric pressure (at atmospheric pressure), for example, by pressing from the support side with a hot pressing member. The pressing condition of the smoothing process can be the same as the condition of the hot pressing of the lamination. The smoothing process can be performed by a commercially available laminator. The lamination and smoothing process may be performed continuously using the above-described commercially available vacuum laminator.

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

In the step (II), the resin composition layer is thermally cured to form an insulating layer. The conditions of the thermosetting of the resin composition layer are not particularly limited, and the conditions employed in forming the insulating layer of the circuit board can be arbitrarily adopted.

The thermosetting condition of the resin composition layer varies depending on, for example, the type of the resin composition. The curing temperature of the resin composition layer is usually in the range of 120 캜 to 240 캜 (preferably in the range of 150 캜 to 220 캜, more preferably in the range of 170 캜 to 200 캜). The curing time is usually in the range of 5 minutes to 120 minutes (preferably 10 minutes to 100 minutes, more preferably 15 minutes to 90 minutes).

The resin composition layer may be preheated to a temperature lower than the curing temperature before thermosetting the resin composition layer. For example, before the resin composition layer is thermally cured, the resin composition layer is heated to a temperature of generally 50 ° C or more and less than 120 ° C (preferably 60 ° C or more and 110 ° C or less, more preferably 70 ° C or more and 100 ° C or less) May be preliminarily heated for usually 5 minutes or more (preferably 5 minutes to 150 minutes, more preferably 15 minutes to 120 minutes).

The manufacturing method of the circuit board may further include (III) a step of piercing the insulating layer, (IV) a step of roughening the insulating layer, and (V) a step of forming a conductor layer. These steps (III) to (V) may be carried out according to a suitable method used in the production of a circuit board. When the support is removed after the step (II), the removal of the support is carried out between the steps (II) and (III), between the steps (III) and (IV) The present invention is not limited thereto.

Step (III) is a step of perforating the insulating layer. Through holes, holes such as via holes and through holes can be formed in the insulating layer. The step (III) can be carried out by, for example, a method such as drilling, laser or plasma, depending on the composition of the resin composition used for forming the insulating layer. The dimensions and shape of the holes can be determined appropriately according to the design of the circuit board.

Step (IV) is a step of applying a roughening treatment to the insulating layer. The order and conditions of the harmonic treatment are not particularly limited, and any order and conditions used in forming the insulating layer of the circuit board can be employed. For example, swelling treatment with a swelling liquid, coarsening treatment with an oxidizing agent, and neutralization treatment with a neutralizing liquid can be carried out in this order to roughen the insulating layer.

The swelling liquid includes, for example, an alkali solution and a surfactant solution, and preferably an alkali solution. As the alkali solution, a sodium hydroxide solution or a potassium hydroxide solution is more preferable. Examples of commercially available swelling liquids include Swelling Dip Siculgans P and Swelling Dip Siculgans SBU manufactured by Atotech Japan Co., Ltd. The swelling liquid may be used alone or in combination of two or more. The swelling treatment by the swelling liquid is not particularly limited. The swelling treatment can be performed, for example, by immersing the insulating layer in a swelling solution at 30 캜 to 90 캜 for 1 minute to 20 minutes. From the viewpoint of suppressing the swelling of the resin in the insulating layer to an appropriate level, it is preferable to immerse the insulating layer in the swelling liquid at 40 占 폚 to 80 占 폚 for 5 minutes to 15 minutes.

As the oxidizing agent, there can be mentioned, for example, an alkaline permanganic acid solution obtained by dissolving potassium permanganate or sodium permanganate in an aqueous solution of sodium hydroxide. The oxidizing agent may be used singly or in combination of two or more kinds. The roughening treatment with an oxidizing agent such as an alkaline permanganic acid solution is preferably carried out by immersing the insulating layer in an oxidizing agent solution heated at 60 캜 to 80 캜 for 10 minutes to 30 minutes. The concentration of the permanganate in the alkaline permanganic acid solution is preferably 5% by mass to 10% by mass. Examples of commercially available oxidizing agents include alkaline permanganic acid solutions such as "Concentrate Compact CP" manufactured by Atotech Japan Co., Ltd. and "Dozing Solution · Securigans P".

As the neutralizing solution, an acidic aqueous solution is preferable. As a commercial product of the neutralization liquid, for example, "Reduction Solution · Securigans P" manufactured by Atotech Japan Co., Ltd. can be mentioned. The neutralizing liquid may be used singly or in combination of two or more kinds. The treatment with the neutralizing liquid can be performed by immersing the treated surface of the insulating layer subjected to the roughening treatment with an oxidizing agent in a neutralizing solution at 30 ° C to 80 ° C for 5 minutes to 30 minutes. It is preferable to immerse the insulating layer subjected to the roughening treatment with an oxidizing agent in a neutralizing solution at 40 캜 to 70 캜 for 5 minutes to 20 minutes in terms of workability and the like.

Step (V) is a step of forming a conductor layer. The material used for the conductor layer is not particularly limited. In a preferred embodiment, the conductor layer comprises at least one metal 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 the alloy layer include a layer formed of an alloy of two or more metals selected from the above-mentioned group (for example, a nickel-chromium alloy, a copper-nickel alloy, and a copper-titanium alloy). Among them, chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver or a copper single metal layer is preferable from the viewpoints of general versatility of the conductor layer, cost and ease of patterning. Or an alloy layer of a nickel-chromium alloy, a copper-nickel alloy, or a copper-titanium alloy. In addition, chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver or copper single metal layers; Alternatively, a nickel-chromium alloy alloy layer is more preferable, and a copper alloy layer is more preferable.

The conductor layer may have a single-layer structure or may have a multi-layer structure including two or more single metal layers or alloy layers made of different kinds of metals or alloys. When the conductor layer is a multilayer 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 is usually from 3 to 200 mu m, preferably from 10 to 100 mu m.

The conductor layer can be formed, for example, by directly patterning it using a metal foil used as a support for an adhesive film. The conductor layer can be formed by, for example, plating. As a forming method by plating, a conductor layer having a desired wiring pattern can be formed by plating the surface of the insulating layer by a method such as a semiadditive method or a pull additive method. Above all, from the viewpoint of simplicity of production, it is preferable to form it by the semi-additive method.

Hereinafter, an example of forming the conductor layer by the semi-additive method will be described. First, a plating seed layer is formed on the surface of the insulating layer by electroless plating. Subsequently, a mask pattern is formed on the formed plating seed layer to expose a part of the plating seed layer so as to correspond to the desired wiring pattern. A metal layer is formed on the exposed plating seed layer by electrolytic plating, and then the mask pattern is removed. Thereafter, an unnecessary plating seed layer is removed by etching or the like, and a conductor layer having a desired wiring pattern can be formed.

The conductor layer may be formed using, for example, a metal foil. When the conductive layer is formed using a metal foil, it is preferable that the step (V) is carried out between the step (I) and the step (II). For example, after the step (I), the support is removed and a metal foil is laminated on the surface of the exposed resin composition layer. The lamination of the resin composition layer and the metal foil can be carried out by a vacuum laminating method. The lamination conditions may be the same as the lamination conditions of the inner layer substrate and the adhesive film in the step (I). Subsequently, an insulating layer is formed by carrying out the step (II). Thereafter, the metal layer on the insulating layer can be used to form a conductor layer having a desired wiring pattern by a subtractive method, a modified semi-additive method or the like. The metal foil can be produced by, for example, an electrolytic method, a rolling method, or the like. Examples of commercial products of metal foil include HLP foil, JXUT-III foil, 3EC-III foil, and TP-III foil manufactured by JX Nikkosuke Kikuchi Kogyo Co., Ltd., and the like.

When the circuit board has two or more insulating layers and a conductor layer (build-up layer), the above-described step of forming the insulating layer and the step of forming the conductor layer are repeated one or more times, A circuit board having a multilayer wiring structure can be manufactured.

In another embodiment, the circuit board can be made using a prepreg instead of an adhesive film. The manufacturing method using the prepreg is basically the same as the case of using the adhesive film.

[16. Semiconductor device]

The semiconductor device includes the circuit board. This semiconductor device can be manufactured by using a circuit board.

Examples of the semiconductor device include various semiconductor devices provided in an electric product (such as a computer, a mobile phone, a digital camera and a television) and a vehicle (such as a motorcycle, a car, a train, have.

The semiconductor device can be manufactured, for example, by mounting a component (semiconductor chip) in a conductive portion of a circuit board. The " conduction point " is a " position at which an electric signal is transmitted from the circuit board ", and the position of the conduction point may be the surface of the circuit board or the portion embedded in the circuit board. Further, the semiconductor chip can be arbitrarily used as an electric circuit element made of a semiconductor.

The semiconductor chip mounting method in manufacturing the semiconductor device can employ any method in which the semiconductor chip effectively functions. Examples of the semiconductor chip mounting method include a wire bonding mounting method, a flip chip mounting method, a mounting method using a bumpless buildup layer (BBUL), a mounting method using an anisotropic conductive film (ACF) As shown in Fig. Here, the " mounting method using the bumpless buildup layer (BBUL) " means a mounting method in which " the semiconductor chip is directly buried in the circuit board to connect the semiconductor chip and the circuit board wiring.

[Example]

Hereinafter, the present invention will be described concretely with reference to Examples, but the present invention is not limited to these Examples. In the following description, " part " and "% " mean " part by mass " and "% by mass ", respectively, unless otherwise specified.

[Example 1]

, 20 parts of a liquid bisphenol A type epoxy resin (epoxy equivalent 187, "jER828US" manufactured by Mitsubishi Chemical Corporation), 10 parts of a biscylsilol type epoxy resin (epoxy equivalent 190, "YX4000HK" manufactured by Mitsubishi Chemical Corporation) , 10 parts of a naphthol type epoxy resin (epoxy equivalent 332, " ESN475V " manufactured by Shinnitetsu Sumikin Chemical Co., Ltd.), and 30 parts of a phenoxy resin (nonvolatile component 30% 20 parts of methyl ethyl ketone / cyclohexanone = 1/1 solution, "YL7553BH30" manufactured by Mitsubishi Chemical Corporation) was dissolved by heating in 60 parts of methyl ethyl ketone and 20 parts of cyclohexanone with stirring to obtain a resin solution.

To this resin solution were added 11 parts of a carbodiimide compound (toluene solution of a non-volatile component 50% by mass, "V-03" manufactured by Nissinbo Chemical Co., Ltd.) 100 parts of spherical silica ("SO-C2" manufactured by Adomex Co., Ltd., average particle diameter 0.5 μm, specific surface area 5.9 m ² / g) surface-treated with polytetrafluoroethylene particles , 10 parts of an active ester curing agent (active equivalent weight 223, toluene solution of a nonvolatile component of 65 mass%, " HPC8000-65T ", manufactured by DIC Corp.), 80 parts of triazine 20 parts of skeleton-containing cresol novolak type curing agent (phenol equivalent 151, 2-methoxypropanol solution of nonvolatile component 50 mass%, " LA3018-50P ", manufactured by DIC Corporation), 20 parts of a curing accelerator (4-dimethylaminopyridine 4 parts by mass of a non-volatile component (5% by mass of methyl ethyl ketone solution), and 4 parts by volume of a non-particulate fluoropolymer Chemical Co., Ltd., "LE-605") were mixed with 4 parts, and obtain a resin varnish was uniformly dispersed in a high-speed rotary mixer.

As a support, a polyethylene terephthalate film (thickness: 38 mu m, "AL5" manufactured by LINTEX Co., Ltd.) having an aliquot resin-based release layer was prepared. On the support, the resin varnish was uniformly coated using a die coater. The applied resin varnish was dried at 80 to 120 캜 (average 100 캜) for 6 minutes to form a resin composition layer, and an adhesive film having a support and a resin composition layer was obtained. The thickness of the resin composition layer was 50 mu m, and the amount of the residual solvent in the resin composition was about 2 mass%.

Subsequently, while the polypropylene film having a thickness of 15 占 퐉 was bonded to the surface of the resin composition layer, the adhesive film was rolled up. The wound adhesive film was slit at a width of 507 mm to obtain a sheet-like adhesive film having a size of 507 mm x 336 mm.

[Example 2]

80 parts of polytetrafluoroethylene particles ("LEBRON L-2" manufactured by Daikin Industries, Ltd.) were changed to 80 parts of polytetrafluoroethylene particles ("KTL-500F" manufactured by Kitamura, average particle diameter 0.3 μm). A resin varnish and an adhesive film were prepared in exactly the same manner as in Example 1 except for the above.

[Example 3]

100 parts of spherical silica (" SO-C2 " manufactured by Adomex Co., Ltd.) surface-treated with N-phenyl-3-aminopropyltrimethoxysilane (KBM573 manufactured by Shinetsu Kagaku Co., Ltd.) and 100 parts of polytetrafluoroethylene particles ) Was changed to 170 parts of polytetrafluoroethylene particles (" KTL-500F " manufactured by Kitamura Co., Ltd., average particle diameter 0.3 mu m). A resin varnish and an adhesive film were prepared in exactly the same manner as in Example 1 except for the above.

[Example 4]

The amount of the active ester type curing agent (toluene solution of a nonvolatile component of 65 mass%, " HPC8000-65T ", manufactured by DIC Corporation) was changed from 10 parts to 15 parts. Further, the amount of the carbodiimide compound ("V-03" manufactured by Nissinbo Chemical Co., Ltd., toluene solution of a non-volatile component of 50 mass%) was changed from 11 parts to 2 parts. A resin varnish and an adhesive film were prepared in exactly the same manner as in Example 1 except for the above.

[Example 5]

80 parts of polytetrafluoroethylene particles ("LEBRON L-2" manufactured by Daikin Industries, Ltd.) and 4 parts of fluoropolymer ("LE-605" manufactured by Kyowa Chemical Industry Co., Ltd.) were mixed in advance and mixed in a resin solution. A resin varnish and an adhesive film were prepared in exactly the same manner as in Example 1 except for the above.

[Example 6]

30 parts of biphenylaralkyl type epoxy resin ("NC3000" manufactured by Nippon Kayaku Co., Ltd.) was changed to 27 parts of naphthylene ether type epoxy resin (epoxy equivalent 260, "HP6000" manufactured by DIC Corporation). A resin varnish and an adhesive film were prepared in exactly the same manner as in Example 1 except for the above.

[Example 7]

20 parts of a naphthylene ether type epoxy resin (epoxy equivalent 260, "HP6000" manufactured by DIC Corporation) and 30 parts of a naphthalene type tetrafunctional epoxy resin (epoxy equivalent 163 , &Quot; HP4700 ", manufactured by DIC Corporation). A resin varnish and an adhesive film were prepared in exactly the same manner as in Example 1 except for the above.

[Example 8]

20 parts of a triazine skeleton-containing cresol novolak type curing agent ("LA3018-50P" manufactured by DIC Corporation, 2-methoxypropanol solution of a nonvolatile component of 50 mass%) was added to 20 parts of a naphthol type curing agent (hydroxyl group equivalent 215, manufactured by Shinnitodezakagaku Co., SN485 ") and 10 parts of triazine-containing phenol novolak resin (hydroxyl equivalent of 125," LA7054 "manufactured by DIC Corporation, MEK solution of 60% nonvolatile component). A resin varnish and an adhesive film were prepared in exactly the same manner as in Example 1 except for the above.

[Example 9]

To the resin varnish, 2 parts of N-phenyl-3-aminopropyltrimethoxysilane (KBM573, Shin-Etsu Chemical Co.) was added. A resin varnish and an adhesive film were prepared in exactly the same manner as in Example 1 except for the above.

[Example 10]

The amount of the active ester type curing agent (toluene solution of a nonvolatile component of 65 mass%, " HPC8000-65T ", manufactured by DIC Corporation) was changed from 10 parts to 5 parts. Further, the amount of the cresol novolak type curing agent containing triazine skeleton ("LA3018-50P" manufactured by DIC Corporation, 2-methoxypropanol solution of 50 mass% non-volatile component) was changed from 20 parts to 5 parts. Further, the amount of the carbodiimide compound ("V-03" manufactured by Nissinbo Chemical Co., Ltd., toluene solution of a non-volatile component of 50 mass%) was changed from 11 parts to 35 parts. A resin varnish and an adhesive film were prepared in exactly the same manner as in Example 1 except for the above.

[Comparative Example 1]

The amount of the active ester type curing agent (toluene solution of a nonvolatile component of 65 mass%, "HPC8000-65T" manufactured by DIC Corporation) was changed from 10 parts to 20 parts. Further, the amount of the carbodiimide compound ("V-03" manufactured by Nissinbo Chemical Co., Ltd., toluene solution of the non-volatile component of 50 mass%) was changed from 11 parts to 0 part. A resin varnish and an adhesive film were prepared in exactly the same manner as in Example 1 except for the above.

[Measurement of dielectric constant]

A polyethylene terephthalate film ("PET501010" manufactured by Lintec Corp.) having a surface subjected to release treatment was prepared. On this polyethylene terephthalate film, resin varnishes obtained in Examples and Comparative Examples were uniformly coated using a die coater so that the thickness of the resin composition layer after drying was 50 占 퐉. The coated resin varnish was dried at 80 캜 to 110 캜 (average 95 캜) for 6 minutes to obtain a resin composition layer. Thereafter, the resin composition layer was heat-treated at 200 캜 for 90 minutes to cure, and the support was peeled off to obtain a cured film formed of the cured product of the resin composition. The cured film was cut into a length of 80 mm and a width of 2 mm, and an evaluation sample was obtained.

The dielectric sample of the cured product of the resin composition was measured for the evaluation sample at a measurement frequency of 5.8 GHz and a measurement temperature of 23 占 폚 by a cavity resonance perturbation method using an analyzer ("HP8362B" manufactured by Agilent Technologies) . The measurement was carried out on two test pieces, and an average value thereof was calculated.

[Measurement of glass transition temperature]

The cured film was cut to a width of about 5 mm and a length of about 15 mm to obtain a test piece. The test piece was subjected to thermomechanical analysis by a tensile weighting method using a thermomechanical analyzer ("Thermo Plus TMA8310" manufactured by Rigaku Corporation). Specifically, after inserting the test piece into the thermomechanical analyzer, analysis was carried out twice successively under the conditions of a load of 1 g and a temperature raising rate of 5 캜 / min. Then, in the second measurement, the glass transition temperature (Tg; 占 폚) was calculated.

[Measurement of Peel Strength]

(1) Underlayer Treatment of Inner Layer Substrate:

A glass cloth substrate epoxy resin double-side copper-clad laminate (thickness of copper foil of 18 mu m, substrate thickness of 0.8 mm, "R5715ES" manufactured by Matsushita Electric KK) on which an inner layer circuit was formed was prepared as an inner layer substrate. Both surfaces of this inner layer substrate were etched with a thickness of 1 mu m with an etching agent (" CZ8100 " manufactured by McCarthy Co., Ltd.) to perform coarsening of copper surfaces on both inner layer substrates.

(2) Adhesive film Laminate:

The adhesive films prepared in Examples and Comparative Examples were laminated on both surfaces of the inner layer substrate so that the resin composition layer was in contact with the inner layer substrate using a vacuum type vacuum laminator (CVP700, two stage built-up laminator manufactured by Nikko Material ≪ / RTI > The laminate was decompressed for 30 seconds to adjust the air pressure to 13 hPa or less, followed by compression at 100 DEG C and a pressure of 0.74 MPa for 30 seconds. Then, hot pressing was performed at 100 占 폚 and a pressure of 0.5 MPa for 60 seconds.

(3) Curing of resin composition:

The adhesive film laminated on the inner layer substrate was heated at 100 캜 for 30 minutes and further at 180 캜 for 30 minutes to thermally cure the resin composition layer to form an insulating layer. Thereafter, the polyethylene terephthalate film as a support was peeled off. Thus, a sample substrate having an insulating layer, an inner layer substrate and an insulating layer in this order was obtained.

(4) Harmonizing treatment:

The sample substrate was immersed in a swelling solution ("Swelling Deep Sucuregent P" manufactured by Atotech Japan Co., Ltd., containing diethylene glycol monobutyl ether) at 60 ° C for 10 minutes. Subsequently, the sample substrate was immersed in a coagulating solution ("Concentrate Compact P" manufactured by Atotech Japan Co., Ltd., KMnO ₄ : 60 g / L, NaOH: 40 g / L aqueous solution) at 80 ° C for 20 minutes. Next, the sample substrate was immersed in a neutralizing solution ("Reduction Solution · Securigant P" manufactured by Atotech Japan Co., Ltd.) at 40 ° C for 5 minutes. Thereafter, the sample substrate was dried at 80 DEG C for 30 minutes to obtain a coherent substrate. The arithmetic average roughness (Ra value) and the 10-point average roughness (Rz value) of the surface of the insulating layer of the coarse substrate were measured by a method described later.

(5) Plating by semi-additive method:

The coarsened substrate was immersed in a solution for electroless plating containing PdCl ₂ at 40 ° C for 5 minutes and then immersed in an electroless copper plating solution at 25 ° C for 20 minutes. Thereafter, the coarsened substrate was annealed at 150 캜 for 30 minutes. An etching resist was formed on the roughened substrate after the annealing, and a pattern was formed by etching. Thereafter, copper sulfate electroplating was performed to form a conductor layer with a thickness of 25 mu m on the surface of the insulating layer. Subsequently, annealing was performed at 180 캜 for 30 minutes to obtain a circuit board having a conductor layer on the insulating layer.

(6) Measurement of Peel Strength (Peel Strength) of Plated Conductor Layer:

The conductor layer of the circuit board was cut so as to surround a rectangular portion having a width of 10 mm and a length of 100 mm. One end in the longitudinal direction of this rectangular portion was peeled off and picked up by a gripping tool (AC-50CSL manufactured by TSE). Then, a peel test was conducted to peel the conductor layer in a direction perpendicular to the surface of the circuit board at a rate of 50 mm / min at room temperature, and the load (kgf / cm) when the length was peeled off was measured as the peel strength .

[Measurement of Peel Strength after HAST Test]

The above-mentioned circuit board was subjected to an accelerated environmental test as a HAST test in which it was exposed to an environment at a temperature of 130 DEG C and a humidity of 85% RH for 100 hours by using an advanced accelerated life testing apparatus ("PM422" manufactured by Gusumoto Chemical Industry Co., Ltd.). Thereafter, the peel strength at the time when the conductor layer of the circuit board was peeled off was measured by the same operation as the above-mentioned [Measurement of Peel Strength] (Step 6) " Measurement of Peel Strength (Peel Strength) of Plated Conductor Layer & .

(F ₀ -F ₁ ) / F ₀ } × 100 (%) of the peel strength by the acceleration environmental test from the peel strength (F ₀ ) before the accelerated environmental test and the peel strength (F ₁ ) ) Was calculated. Good "was judged as the rate of decrease of 30% or less, and" Good "was judged as being larger than 30%.

[Evaluation of breaking point shindo]

The cured film was subjected to a tensile test in accordance with Japanese Industrial Standards (JIS K7161) using a tensile tensile tester (manufactured by A & D Co.) at a temperature of 25 ° C, a humidity of 40% RH and a tensile speed of 50 mm / , And the elongation at break of the sample was measured.

[Measurement of arithmetic mean roughness (Ra) and ten-point average roughness (Rz) of insulating layer surface]

The arithmetic mean roughness (Ra) and the 10-point average roughness (Rz) of the surface of the insulating layer of the coarse substrate were measured using a VSI contact mode, a 50x lens By a numerical value obtained by setting the measurement range to 121 mu m x 92 mu m. The average value of 10 randomly selected points was obtained and used as a measurement value.

[result]

The results of the above-described examples and comparative examples are shown in the following table. In the following table, the amount of each component represents the mass part of the non-volatile component.

[Table 1. Results of Examples and Comparative Examples]

[Review]

As can be seen from Table 1, low permittivity is obtained in any of the embodiments. Further, in Examples, the glass transition temperature (Tg) can be increased and the rate of decrease of the peel strength after the HAST test can be made smaller than that of Comparative Example 1 in which the carbodiimide compound (B) is not used . From these results, it was confirmed that the present invention can realize a resin composition capable of suppressing the lowering of the adhesiveness to the conductor layer due to the HAST test with a low dielectric constant and obtaining an insulating layer having a high glass transition temperature .

In Examples 1 to 10, breaking point elongation and surface roughness were obtained to the same extent as in Comparative Example 1. [ Therefore, it can be seen that the insulating layer obtained by the present invention has excellent characteristics in terms of elongation at break and surface roughness of the same level as that of the conventional product.

Compared with Example 10 in which a large amount of the carbodiimide compound (B) is used, the elongation at break can be increased in the other Examples 1 to 9. From these results, it was confirmed that there is an appropriate range for the amount of the (B) carbodiimide compound from the viewpoint of obtaining an insulating layer excellent in mechanical strength.

In the fifth embodiment, the surface roughness of the insulating layer can be made smaller than that of the first embodiment. From this result, it is found that the non-particulate (G) component is mixed with the fluorine-containing filler (C-1), and the fluorine-containing filler is mixed with the fluorine-containing filler in order to obtain an insulating layer having a low surface roughness by increasing the dispersibility of the fluorine- It is preferable to mix the components with other components.

In the ninth embodiment, the surface roughness of the insulating layer can be made smaller than that in the first embodiment. From this result, it can be seen that it is preferable to use the coupling agent (H) from the viewpoint of increasing the dispersibility of the inorganic filler (C-2) and obtaining an insulating layer having a small surface roughness.

In the above examples, it was confirmed that even when the components (D) and (H) were not used, the results were the same as those of the above-mentioned examples although there were differences in the degree.

Claims (13)

A resin composition comprising (A) an epoxy resin, (B) a carbodiimide compound, and (C) a filler,
(C) comprises (C-1) a fluorine-based filler,
Wherein the amount of the component (C) is 30% by mass to 80% by mass with respect to 100% by mass of the nonvolatile component in the resin composition. The resin composition according to claim 1, wherein the component (C-1) is a fluorine-based polymer particle. The resin composition according to claim 1, wherein the component (C-1) is a polytetrafluoroethylene particle. The resin composition according to claim 1, wherein the amount of the component (B) is 0.5% by mass to 15% by mass based on 100% by mass of the resin component in the resin composition. The positive resist composition according to claim 1, wherein component (C) comprises (C-2) an inorganic filler,
Wherein the amount of the component (C-2) is 5% by mass or more and 70% by mass or less based on 100% by mass of the nonvolatile component in the resin composition. The resin composition according to claim 1, wherein the amount of the component (C-1) is 5% by mass or more and 80% by mass or less based on 100% by mass of the nonvolatile component in the resin composition. The epoxy resin composition according to claim 1, wherein the component (A) is at least one selected from the group consisting of bisphenol A epoxy resin, biquileneol epoxy resin, biphenylaralkyl epoxy resin, naphthylene ether epoxy resin, naphthalene type tetrafunctional epoxy resin and naphthol epoxy resin And at least one epoxy resin selected from the group consisting of epoxy resins. The resin composition according to claim 1, wherein the component (C-1) has an average particle diameter of 0.05 탆 or more and 10 탆 or less. The resin composition according to claim 1, comprising an active ester-based curing agent. The resin composition according to claim 1, which is used for forming an insulating layer of a circuit board. A sheet-stacked material comprising the resin composition according to any one of claims 1 to 10. A circuit board comprising an insulating layer made of a cured product of the resin composition according to any one of claims 1 to 10. A semiconductor device comprising the circuit board according to claim 12.