JP2024008617A - Molding resin composition, dielectric substrate, and microstrip antenna - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide techniques regarding a molding resin composition capable of realizing a high dielectric constant and a low dielectric loss tangent.

SOLUTION: The molding resin composition includes an epoxy resin (A), a curing agent (B), a high dielectric constant filler (C), and an indene resin (D) having a structural unit represented by the formula (D1) in the figure. (In the formula (D1), R¹ to R⁷ are each independently hydrogen or an organic group in which the number of carbon atoms is from 1 to 3 inclusive.)

SELECTED DRAWING: None

COPYRIGHT: (C)2024,JPO&INPIT

Description

The present invention relates to a molding resin composition, a dielectric substrate, and a microstrip antenna. More specifically, the present invention relates to a molding resin composition, a cured product thereof, a dielectric substrate and a microstrip antenna using the same.

In recent years, wireless communication has become faster, and there is a demand for higher performance and smaller size of the communication equipment used. Furthermore, in recent years, the capacity of wireless communication has increased rapidly, and as a result, the frequencies used for transmission signals are rapidly becoming wider and higher in frequency. For this reason, the frequency band used by communication equipment cannot be supported by the conventional microwave band alone, and is being expanded to include the millimeter wave band. Against this background, there is a strong demand for higher performance antennas installed in communication equipment.

Communication equipment can be further miniaturized if the dielectric constant of the antenna material (dielectric substrate) built into the communication equipment increases. Furthermore, when the dielectric loss tangent of the dielectric substrate becomes smaller, the loss becomes lower, which is advantageous for higher frequencies. Therefore, if a dielectric substrate with a high dielectric constant and a small dielectric loss tangent can be used, it is possible to achieve higher frequencies, thereby shortening the circuit length and downsizing the communication equipment.

Patent Document 1 describes a laminate of a dielectric substrate made of a composite material containing a fluororesin and a glass cloth, and an antenna whose surface in contact with the fluororesin has a two-dimensional roughness Ra of less than 0.2 μm. An antenna having a substrate is disclosed. This document describes the dielectric constant and dielectric loss tangent of a circuit board measured at 1 GHz.

Patent Document 2 discloses a resin composition that includes a siloxane-modified polyamideimide resin, a high dielectric constant filler, and an epoxy resin, and has a cured product having a dielectric constant of 15 or more at 25° C. and 1 MHz. Examples of this document describe an example in which barium titanate is used as the high dielectric constant filler.

Patent Document 3 discloses a resin composition containing an epoxy resin, a dielectric powder, a nonionic surfactant, and an active ester curing agent. This document states that this resin composition can be used as a high dielectric constant insulating material for electronic components used in a high frequency region and a high dielectric constant insulating material for fingerprint sensors. The example of this document describes an example in which barium titanate is used as the dielectric powder.

Patent Document 4 includes an epoxy resin, a curing agent, and an inorganic filler containing predetermined amounts of calcium titanate particles and strontium titanate particles, the inorganic filler consisting of silica particles and alumina particles. Disclosed is a molding resin composition which further contains at least one member selected from the group consisting of:

JP 2018-41998 Publication Japanese Patent Application Publication No. 2004-315653 JP 2020-105523 Publication Patent No. 6870778

In recent years, the technical level required for various properties of high dielectric constant resin compositions has become higher and higher, and even the molding resin compositions and dielectric substrates described in Patent Documents 1 to 4 have high dielectric constants. There was room for improvement in terms of achieving both high and low dielectric loss tangent. Among these, it was remarkable in that it achieved a high dielectric constant and a low dielectric loss tangent while maintaining good mechanical strength when used in antenna structures.

The present inventor focused on the development of a new material that achieves a high dielectric constant and a low dielectric loss tangent, and as a result of conducting studies, discovered that it is effective to use an indene oligomer having a specific structure.

According to the present invention, the following techniques regarding a molding resin composition, a dielectric substrate, and a microstrip antenna are provided.

（一般式（Ｄ１）中、Ｒ^１からＲ^７はそれぞれ独立して、水素または炭素数１以上３以下の有機基を表す。）
［２］ ［１］に記載の成形用樹脂組成物であって、
当該成形用樹脂組成物の硬化物の１ＭＨｚにおける誘電率（Ｄｋ：εｒ）が１０～３０であり、当該成形用樹脂組成物の硬化物の１ＭＨｚにおける誘電正接（Ｄｆ：ｔａｎδ）が０．００２０～０．００５０である、成形用樹脂組成物。
［３］ ［１］または［２］に記載の成形用樹脂組成物であって、
以下の手順で測定される２６０℃での曲げ弾性率が、５０Ｎ／ｍｍ^２ＭＰａ以上である、成形用樹脂組成物。
（手順）当該成形用樹脂組成物を、金型温度１３０℃、注入圧力９．８ＭＰａ、硬化時間３００秒の条件で金型に注入成形したのち、１７５℃、４時間の条件で後硬化させて試験片を作製する。当該試験片を用いて、ＪＩＳ Ｋ ６９１１に準拠して、２６０℃での曲げ弾性率を測定する。
［４］ ［１］乃至［３］いずれか一つに記載の成形用樹脂組成物であって、
前記インデン樹脂（Ｄ）の含有量が、前記エポキシ樹脂（Ａ）１００質量部に対して、４質量部以上５０質量部以下である、成形用樹脂組成物。
［５］ ［１］乃至［４］いずれか一つに記載の成形用樹脂組成物であって、
前記インデン樹脂（Ｄ）の重量平均分子量Ｍｗは４００～４０００である、成形用樹脂組成物。
［６］ ［１］乃至［５］いずれか一つに記載の成形用樹脂組成物であって、
前記インデン樹脂（Ｄ）中の前記一般式（Ｄ１）で示される構造単位のモル含有量が５０％以上である、成形用樹脂組成物。
［７］ ［１］乃至［６］いずれか一つに記載の成形用樹脂組成物であって、
前記高誘電率充填剤（Ｃ）がチタン酸カルシウム、チタン酸バリウム、チタン酸ストロンチウム、チタン酸マグネシウム、ジルコン酸マグネシウム、ジルコン酸ストロンチウム、チタン酸ビスマス、チタン酸ジルコニウム、チタン酸亜鉛、ジルコン酸バリウム、チタン酸ジルコン酸カルシウム、チタン酸ジルコン酸鉛、ニオブ酸マグネシウム酸バリウム、およびジルコン酸カルシウムからなる群より選ばれる１種または２種以上を含む、成形用樹脂組成物。
［８］ ［１］乃至［７］いずれか一つに記載の成形用樹脂組成物であって、
前記高誘電率充填剤（Ｃ）の含有量は、前記成形用樹脂組成物全量に対して、５０～９０質量％である、成形用樹脂組成物。
［９］ ［１］乃至［８］いずれか一つに記載の成形用樹脂組成物であって、
１７５℃におけるゲルタイムが３０～１００秒である、成形用樹脂組成物。
［１０］ ［１］乃至［９］いずれか一つに記載の成形用樹脂組成物であって、
前記エポキシ樹脂（Ａ）は、ビスフェノールＡ型エポキシ樹脂、ビスフェノールＦ型エポキシ樹脂、ビフェニルアラルキル型エポキシ樹脂、ナフタレン型エポキシ樹脂、ジナフトールアラルキル型エポキシ樹脂、ジシクロペンタジエン型エポキシ樹脂、およびグリシジルアミン型エポキシ樹脂の中から選ばれる１種または２種以上を含む、成形用樹脂組成物。
［１１］ ［１］乃至［１０］いずれか一つに記載の成形用樹脂組成物であって、
硬化剤（Ｂ）が、活性エステル系硬化剤および／またはフェノール系硬化剤を含む、成形用樹脂組成物。
［１２］ ［１］乃至［１１］いずれか一つに記載の成形用樹脂組成物であって、
カップリング剤（Ｅ）をさらに含む、成形用樹脂組成物。
［１３］ ［１］乃至［１２］いずれか一つに記載の成形用樹脂組成物であって、
硬化触媒（Ｆ）をさらに含む、成形用樹脂組成物。
［１４］ ［１］乃至［１３］いずれか一つに記載の成形用樹脂組成物であって、
アンテナを形成する材料として用いられる、成形用樹脂組成物。
［１５］ ［１］乃至［１３］いずれか一つに記載の成形用樹脂組成物の硬化物。
［１６］ ［１］乃至［１３］いずれか一つに記載の成形用樹脂組成物を硬化してなる誘電体基板。
［１７］ ［１６］に記載の誘電体基板と、
前記誘電体基板の一方の面に設けられた放射導体板と、
前記誘電体基板の他方の面に設けられた地導体板と、
を備える、マイクロストリップアンテナ。 [1] A molding resin composition containing an epoxy resin (A), a curing agent (B), a high dielectric constant filler (C), and an indene resin (D) having a structural unit represented by the following general formula (D1) thing.

(In general formula (D1), R ¹ to R ⁷ each independently represent hydrogen or an organic group having 1 to 3 carbon atoms.)
[2] The molding resin composition according to [1],
The dielectric constant (Dk: εr) at 1 MHz of the cured product of the molding resin composition is 10 to 30, and the dielectric loss tangent (Df: tan δ) at 1 MHz of the cured product of the molding resin composition is 0.0020 to 0.0020. 0.0050, a molding resin composition.
[3] The molding resin composition according to [1] or [2],
A molding resin composition having a flexural modulus of elasticity at 260° C. of 50 N/mm ² MPa or more as measured by the following procedure.
(Procedure) The molding resin composition was injected into a mold at a mold temperature of 130°C, an injection pressure of 9.8 MPa, and a curing time of 300 seconds, and then post-cured at 175°C for 4 hours. Prepare a test piece. Using the test piece, the flexural modulus at 260°C is measured in accordance with JIS K 6911.
[4] The molding resin composition according to any one of [1] to [3],
A resin composition for molding, wherein the content of the indene resin (D) is 4 parts by mass or more and 50 parts by mass or less, based on 100 parts by mass of the epoxy resin (A).
[5] The molding resin composition according to any one of [1] to [4],
A molding resin composition, wherein the indene resin (D) has a weight average molecular weight Mw of 400 to 4,000.
[6] The molding resin composition according to any one of [1] to [5],
A molding resin composition, wherein the molar content of the structural unit represented by the general formula (D1) in the indene resin (D) is 50% or more.
[7] The molding resin composition according to any one of [1] to [6],
The high dielectric constant filler (C) is calcium titanate, barium titanate, strontium titanate, magnesium titanate, magnesium zirconate, strontium zirconate, bismuth titanate, zirconium titanate, zinc titanate, barium zirconate, A molding resin composition containing one or more selected from the group consisting of calcium zirconate titanate, lead zirconate titanate, barium magnesium niobate, and calcium zirconate.
[8] The molding resin composition according to any one of [1] to [7],
A molding resin composition in which the content of the high dielectric constant filler (C) is 50 to 90% by mass based on the total amount of the molding resin composition.
[9] The molding resin composition according to any one of [1] to [8],
A molding resin composition having a gel time of 30 to 100 seconds at 175°C.
[10] The molding resin composition according to any one of [1] to [9],
The epoxy resin (A) is a bisphenol A type epoxy resin, a bisphenol F type epoxy resin, a biphenylaralkyl type epoxy resin, a naphthalene type epoxy resin, a dinaphthol aralkyl type epoxy resin, a dicyclopentadiene type epoxy resin, and a glycidylamine type epoxy resin. A molding resin composition containing one or more selected from resins.
[11] The molding resin composition according to any one of [1] to [10],
A molding resin composition in which the curing agent (B) contains an active ester curing agent and/or a phenolic curing agent.
[12] The molding resin composition according to any one of [1] to [11],
A molding resin composition further comprising a coupling agent (E).
[13] The molding resin composition according to any one of [1] to [12],
A molding resin composition further comprising a curing catalyst (F).
[14] The molding resin composition according to any one of [1] to [13],
A molding resin composition used as a material for forming antennas.
[15] A cured product of the molding resin composition according to any one of [1] to [13].
[16] A dielectric substrate obtained by curing the molding resin composition according to any one of [1] to [13].
[17] The dielectric substrate according to [16],
a radiation conductor plate provided on one surface of the dielectric substrate;
a ground conductor plate provided on the other surface of the dielectric substrate;
Microstrip antenna.

According to the present invention, it is possible to provide a technique related to a molding resin composition that can realize a high dielectric constant and a low dielectric loss tangent.

FIG. 1 is a top perspective view schematically showing the microstrip antenna of this embodiment.

Embodiments of the present invention will be described in detail below with reference to the drawings. The drawings are for illustrative purposes only. The shape, size ratio, etc. of each member in the drawings do not necessarily correspond to the actual article.

In the present specification, the notation "a to b" in the description of numerical ranges represents a range from a to b, unless otherwise specified. For example, "1 to 5% by mass" means "1 to 5% by mass". Further, the lower limit value and upper limit value of the numerical range can be arbitrarily combined with the lower limit value and upper limit value of other numerical ranges, respectively.

Each component and material illustrated in this specification may be used alone or in combination of two or more, unless otherwise specified.

The molding resin composition of the present embodiment (hereinafter also referred to as "resin composition") comprises an epoxy resin (A), a curing agent (B), a high dielectric constant filler (C), and the following formula (D1). Contains an indene resin (D) having a structural unit represented by:
According to the resin composition of this embodiment, high dielectric constant and low dielectric loss tangent can be achieved while maintaining good processability as a molding material.

（一般式（Ｄ１）中、Ｒ^１からＲ^７はそれぞれ独立して、水素または炭素数１以上３以下の有機基を表す。）

(In general formula (D1), R ¹ to R ⁷ each independently represent hydrogen or an organic group having 1 to 3 carbon atoms.)

Each component contained in the resin composition of this embodiment will be explained below.

[Epoxy resin (A)]
Epoxy resins (A) include bisphenol A epoxy resin, bisphenol F epoxy resin, tetramethylbisphenol F epoxy resin, bisphenol S epoxy resin, bisphenol E epoxy resin, bisphenol M epoxy resin, and bisphenol P epoxy resin. Resin, bisphenol type epoxy resin such as bisphenol Z type epoxy resin; novolac type epoxy resin such as phenol novolac type epoxy resin, cresol novolac type epoxy resin; biphenyl type epoxy resin, biphenyl aralkyl type epoxy resin, aryl alkylene type epoxy resin, naphthalene type epoxy resin, dinaphthol aralkyl type epoxy resin, anthracene type epoxy resin, phenoxy type epoxy resin, dicyclopentadiene type epoxy resin, glycidylamine type epoxy resin, norbornene type epoxy resin, adamantane type epoxy resin, fluorene type epoxy resin, tri-type epoxy resin Examples include phenylmethane type epoxy resin.
Among these, selected from bisphenol A type epoxy resin, bisphenol F type epoxy resin, biphenylaralkyl type epoxy resin, naphthalene type epoxy resin, dinaphthol aralkyl type epoxy resin, dicyclopentadiene type epoxy resin, and glycidylamine type epoxy resin. It is preferable that one type or two or more types are used.

From the viewpoint of obtaining the effects of the present invention, the content of the epoxy resin (A) may be 3% by mass or more and 20% by mass or less, preferably 7% by mass or more and 12% by mass or less, based on the entire resin composition. can.

[Curing agent (B)]
The curing agent (B) is used to cure the epoxy resin (A). As the curing agent (B), known ones can be used, but it is preferable that the curing agent (B) contains an active ester curing agent (b1) and/or a phenol curing agent (b2).

(Active ester curing agent (b1))
As the active ester curing agent (b1), a compound having one or more active ester groups in one molecule can be used. Among these, active ester curing agents (b1) contain ester groups with high reactivity in one molecule, such as phenol esters, thiophenol esters, N-hydroxyamine esters, and esters of heterocyclic hydroxy compounds. Compounds having two or more are preferred.
In the present embodiment, by including the above-mentioned epoxy resin (A) and the active ester curing agent (b1) in combination, a dielectric substrate excellent in high dielectric constant and low dielectric loss tangent can be obtained.

Preferred specific examples of the active ester curing agent (b1) include an active ester curing agent containing a dicyclopentadiene type diphenol structure, an active ester curing agent containing a naphthalene structure, and an active ester curing agent containing an acetylated product of phenol novolak. Examples of the curing agent include active ester curing agents including benzoylated phenol novolaks, and at least one of them can be included. Among these, active ester curing agents containing a naphthalene structure and active ester curing agents containing a dicyclopentadiene type diphenol structure are more preferable.
Note that "dicyclopentadiene type diphenol structure" refers to a divalent structural unit consisting of phenylene-dicyclopentylene-phenylene.

In this embodiment, the active ester curing agent (b1) can be, for example, a resin having a structure represented by the following general formula (1).

In formula (1), A is a substituted or unsubstituted arylene group connected via an aliphatic cyclic hydrocarbon group, Ar' is a substituted or unsubstituted aryl group, and k is a repeating unit. It is the average value of and ranges from 0.25 to 3.5. B has a structure represented by the following formula (B).

In formula (B), Ar is a substituted or unsubstituted arylene group, and Y is a single bond, a substituted or unsubstituted linear alkylene group having 1 to 6 carbon atoms, or a substituted or unsubstituted carbon atom. These include a cyclic alkylene group of three to six numbers, a substituted or unsubstituted divalent aromatic hydrocarbon group, an ether bond, a carbonyl group, a carbonyloxy group, a sulfide group, or a sulfone group. n is an integer from 0 to 4.

By including the specific active ester curing agent (b1) in the resin composition of the present embodiment, the obtained cured product can have excellent dielectric properties and is excellent in low dielectric loss tangent.

The active ester curing agent (b1) used in the resin composition of this embodiment has an active ester group represented by formula (B).
In the curing reaction between the epoxy resin (A) and the active ester curing agent (b1), the active ester group of the active ester curing agent (b1) reacts with the epoxy group of the epoxy resin (A) to form a secondary hydroxyl group. arise. This secondary hydroxyl group is blocked by the ester residue of the active ester curing agent (b1). Therefore, the dielectric loss tangent of the cured product is reduced.

In one embodiment, the structure represented by the above formula (B) is preferably at least one selected from the following formulas (B-1) to (B-6).

In formulas (B-1) to (B-6),
R ¹ is each independently a hydrogen atom, an alkyl group having 1 to 4 carbon atoms, an alkoxy group having 1 to 4 carbon atoms, a phenyl group, or an aralkyl group; R ² is each independently a hydrogen atom, an alkyl group having 1 to 4 carbon atoms; an alkyl group, an alkoxy group having 1 to 4 carbon atoms, or a phenyl group; n and p are each an integer of 1 to 4.

The structures represented by the above formulas (B-1) to (B-6) are all highly oriented structures, so when an active ester curing agent (b1) containing them is used, the structure obtained The cured product of the resin composition has a low dielectric loss tangent and excellent adhesion to metals, and therefore can be suitably used as a semiconductor encapsulation material.
Among them, from the viewpoint of low dielectric loss tangent, active ester curing agent (b1) having a structure represented by formula (B-3) or (B-5) is preferable, and furthermore, X in formula (B-3) is an ether. More preferred is an active ester curing agent (b1) having a structure that is a bond or a structure in which two carbonyloxy groups are at the 4,4'-positions in formula (B-5). Further, it is preferable that all R ¹ in each formula are hydrogen atoms.

"Ar'" in formula (1) is an aryl group, for example, phenyl group, o-tolyl group, m-tolyl group, p-tolyl group, 3,5-xylyl group, o-biphenyl group, m-biphenyl group. p-biphenyl group, 2-benzylphenyl group, 4-benzylphenyl group, 4-(α-cumyl)phenyl group, 1-naphthyl group, 2-naphthyl group, etc. Among these, 1-naphthyl group or 2-naphthyl group is preferable because a cured product with a lower dielectric loss tangent can be obtained.

In this embodiment, "A" in the active ester curing agent (b1) represented by formula (1) is a substituted or unsubstituted arylene group connected via an aliphatic cyclic hydrocarbon group; Examples of such an arylene group include a structure obtained by polyaddition reaction of an unsaturated aliphatic cyclic hydrocarbon compound containing two double bonds in one molecule and a phenolic compound.

Examples of the unsaturated aliphatic cyclic hydrocarbon compound containing two double bonds in one molecule include dicyclopentadiene, cyclopentadiene polymer, tetrahydroindene, 4-vinylcyclohexene, and 5-vinyl-2-norbornene. , limonene, etc., and each of these may be used alone or two or more types may be used in combination. Among these, dicyclopentadiene is preferred because it provides a cured product with excellent heat resistance. Since dicyclopentadiene is contained in petroleum fractions, industrial dicyclopentadiene may contain cyclopentadiene polymers and other aliphatic or aromatic diene compounds as impurities. However, in consideration of performance such as heat resistance, curability, and moldability, it is desirable to use a product with dicyclopentadiene purity of 90% by mass or more.

On the other hand, the phenolic compounds include, for example, phenol, cresol, xylenol, ethylphenol, isopropylphenol, butylphenol, octylphenol, nonylphenol, vinylphenol, isopropenylphenol, allylphenol, phenylphenol, benzylphenol, chlorophenol, bromophenol, Examples include 1-naphthol, 2-naphthol, 1,4-dihydroxynaphthalene, 2,3-dihydroxynaphthalene, 2,3-dihydroxynaphthalene, 2,6-dihydroxynaphthalene, and 2,7-dihydroxynaphthalene, each of which can be used alone. It may be used or two or more types may be used in combination. Among these, phenol is preferred because it provides an active ester curing agent (b1) with high curability and excellent dielectric properties in a cured product.

In a preferred embodiment, "A" in the active ester curing agent (b1) represented by formula (1) has a structure represented by the following formula (A). A resin composition containing an active ester curing agent (b1) in which "A" in formula (1) has the following structure has a cured product having a low dielectric loss tangent and excellent adhesion to insert products.

In formula (A), R ³ is each independently a hydrogen atom, an alkyl group having 1 to 4 carbon atoms, an alkoxy group having 1 to 4 carbon atoms, a phenyl group, or an aralkyl group, and 1 is 0 or 1. Yes, and m is an integer of 1 or more.

Among the active ester curing agents (b1) represented by formula (1), particularly preferred are those represented by the following formulas (1-1), (1-2), and (1-3). Examples include resins, and among them, resins represented by the following formula (1-3) are preferred.

In formula (1-1), R ¹ and R ³ are each independently a hydrogen atom, an alkyl group having 1 to 4 carbon atoms, an alkoxy group having 1 to 4 carbon atoms, a phenyl group, or an aralkyl group, and Z is a phenyl group, a naphthyl group, or a phenyl group or a naphthyl group having 1 to 3 alkyl groups having 1 to 4 carbon atoms on the aromatic nucleus, l is 0 or 1, and k is the average of the repeating units. Yes, and ranges from 0.25 to 3.5.

In formula (1-2), R ¹ and R ³ are each independently a hydrogen atom, an alkyl group having 1 to 4 carbon atoms, an alkoxy group having 1 to 4 carbon atoms, a phenyl group, or an aralkyl group, and Z is a phenyl group, a naphthyl group, or a phenyl group or a naphthyl group having 1 to 3 alkyl groups having 1 to 4 carbon atoms on the aromatic nucleus, l is 0 or 1, and k is the average of the repeating units. Yes, and ranges from 0.25 to 3.5.

In formula (1-3), R ¹ and R ³ are each independently a hydrogen atom, an alkyl group having 1 to 4 carbon atoms, an alkoxy group having 1 to 4 carbon atoms, a phenyl group, or an aralkyl group. , Z is a phenyl group, a naphthyl group, or a phenyl group or a naphthyl group having 1 to 3 alkyl groups having 1 to 4 carbon atoms on the aromatic nucleus, l is 0 or 1, and k is a repeating unit. It is the average of 0.25 to 3.5.

The active ester curing agent (b1) used in the present invention comprises a phenolic compound having a structure in which a plurality of aryl groups having a phenolic hydroxyl group are linked via an aliphatic cyclic hydrocarbon group, and an aromatic nucleus-containing dicarboxylic acid or It can be produced by a known method of reacting the halide with an aromatic monohydroxy compound.

The reaction ratio of the above-mentioned phenolic compound, aromatic nucleus-containing dicarboxylic acid or its halide, and aromatic monohydroxy compound can be adjusted as appropriate depending on the desired molecular design. Since the active ester curing agent (b1) is obtained, the phenolic hydroxyl group of the phenolic compound is 0.25 per mole of the carboxyl group or acid halide group of the aromatic nucleus-containing dicarboxylic acid or its halide. It is preferable to use each raw material in a proportion such that the amount of hydroxyl group contained in the aromatic monohydroxy compound is in the range of 0.10 to 0.75 mol, and the hydroxyl group contained in the aromatic monohydroxy compound is in the range of 0.10 to 0.75 mol. It is preferable to use each raw material in a ratio such that the phenolic hydroxyl group is in the range of 0.50 to 0.75 mol, and the hydroxyl group possessed by the aromatic monohydroxy compound is in the range of 0.25 to 0.50 mol. preferable.

In addition, the functional group equivalent of the active ester curing agent (b1) is defined as the number of functional groups in the resin, which is the sum of the aryl carbonyloxy groups and phenolic hydroxyl groups in the resin structure. It is preferably in the range of 200 g/eq or more and 230 g/eq or less, and more preferably in the range of 210 g/eq or more and 220 g/eq or less.

In the resin composition of the present embodiment, the content of the active ester curing agent (b1) and the epoxy resin (A) is determined so that a cured product with excellent curability and a low dielectric loss tangent can be obtained. The ratio is preferably such that the amount of epoxy groups in the epoxy resin (A) is 0.8 to 1.2 equivalents per total equivalent of active groups in the agent (b1). Here, the active group in the active ester curing agent (b1) refers to an arylcarbonyloxy group and a phenolic hydroxyl group contained in the resin structure.

In the composition of the present embodiment, the active ester curing agent (b1) is preferably 0.2% by mass or more and 15% by mass or less, more preferably 0.5% by mass or more and 10% by mass, based on the entire resin composition. % or less, more preferably 1.0% by mass or more and 7% by mass or less.
By containing the specific active ester curing agent (b1) in the above range, the obtained cured product can have better dielectric properties and is further excellent in low dielectric loss tangent.

By using the active ester curing agent (b1) in combination with the high dielectric constant filler (C) described below, the resin composition of this embodiment has excellent high dielectric constant and low dielectric loss tangent, and can be used in high frequency bands. is also excellent in these effects.
From the viewpoint of obtaining the above effects, the active ester curing agent (b1) is preferably 1 part by mass or more and 30 parts by mass or less, more preferably 2 parts by mass, based on 100 parts by mass of the high dielectric constant filler (C) described below. It can be contained in an amount of at least 3 parts by mass and at most 20 parts by mass, more preferably at least 3 parts by mass and at most 15 parts by mass.

(Phenol curing agent (b2))
Examples of the phenolic curing agent (b2) include phenol novolak resin, cresol novolac resin, aromatic hydrocarbon formaldehyde resin modified phenol resin, dicyclopentadiene phenol addition type resin, phenol aralkyl resin, naphthol aralkyl resin, trimethylolmethane resin, tetra Phenylolethane resin, naphthol novolak resin, naphthol-phenol co-condensed novolak resin, naphthol-cresol co-condensed novolak resin, biphenyl-modified phenol resin (a polyhydric phenol compound in which phenol nuclei are linked by bismethylene groups), biphenyl-modified naphthol resin ( Examples include polyhydric phenol compounds such as polyhydric naphthol compounds (polyhydric naphthol compounds in which phenol nuclei are linked with bismethylene groups) and aminotriazine-modified phenol resins (polyhydric phenol compounds in which phenol nuclei are linked with melamine, benzoguanamine, etc.).

The content of the phenolic curing agent (b2) is preferably 20% by mass or more and 70% by mass or less based on the epoxy resin (A). By using the curing agent in an amount within the above range, a resin composition having excellent curability can be obtained.

When the curing agent (B) contains an active ester curing agent (b1) and a phenolic curing agent (b2), the ratio of the content of the phenolic curing agent (b2) to the active ester curing agent (b1) is preferably can be 0.5 or more and 8 or less, more preferably 1 or more and 5 or less, and still more preferably 1.5 or more and 3 or less.
By containing the active ester curing agent (b1) and the phenol curing agent (b2) in the above ratio, the resulting cured product can have better dielectric properties and is further excellent in low dielectric loss tangent.

In the composition of the present embodiment, the content of the curing agent (B) containing the active ester curing agent (b1) and/or the phenolic curing agent (b2) is preferably 0. 2% by mass or more and 15% by mass or less, more preferably 0.5% by mass or more and 10% by mass or less, even more preferably 1% by mass or more and 7% by mass or less, even more preferably 2% by mass or more and 6.0% by mass. It is as follows.
By containing the curing agent (B) in the above range, the resulting cured product can have better dielectric properties. Furthermore, by controlling the amount of the curing agent (B) to be less than or equal to the above upper limit, the dielectric loss tangent can be further reduced.

[High dielectric constant filler (C)]
The high dielectric constant filler (C) is used to effectively improve the dielectric constant of the resin composition of this embodiment. The high dielectric constant filler (C) is a filler having a dielectric constant of 30 or more, preferably 70 or more, and more preferably 100 or more. The upper limit of the dielectric constant is not particularly limited, but may be, for example, about 30,000.

The high dielectric constant filler (C) is preferably made of a metal oxide, such as titanium-based metal oxides and zirconia-based metal oxides.
Specifically, the high dielectric constant filler (C) includes calcium titanate, strontium titanate, magnesium titanate, magnesium zirconate, strontium zirconate, bismuth titanate, zirconium titanate, zinc titanate, barium zirconate, One or more selected from calcium zirconate titanate, lead zirconate titanate, barium magnesium niobate, calcium zirconate, and the like can be used.
From the viewpoint of obtaining the effects of the present invention, the high dielectric constant filler (C) is preferably at least one selected from calcium titanate, strontium titanate, and magnesium titanate. More preferred are calcium and magnesium titanate.

The shape of the high dielectric constant filler (C) is not particularly limited, and may be granular, amorphous, flake, or a mixture thereof.
The average particle diameter of the high dielectric constant filler (C) is preferably 0.1 μm or more and 50 μm or less, more preferably 0.5 μm or more, from the viewpoint of obtaining the effects of the present invention and good fluidity and filling properties. It is 20 μm or less, more preferably 1.0 μm or more and 10 μm or less, and even more preferably 1.0 μm or more and 5.0 μm or less.

The content of the high dielectric constant filler (C) is preferably 40% by mass or more, more preferably 50% by mass or more, and still more preferably 60% by mass or more in 100% by mass of the resin composition. The upper limit of the content of the high dielectric constant filler (C) is preferably 80% by mass or less, more preferably 70% by mass or less.
When the content of the high dielectric constant filler (C) is within the above range, the obtained cured product has a high dielectric constant and a low dielectric loss tangent, and is also excellent in producing molded products.

[Indene resin (D)]
The indene resin (D) of the present embodiment has a structural unit derived from so-called indene or an indene derivative, represented by the following formula (D1). Thereby, the dielectric loss tangent of the resin composition can be lowered while maintaining good mechanical properties.

（一般式（Ｄ１）中、Ｒ^１からＲ^７はそれぞれ独立して、水素または炭素数１以上３以下の有機基である。）

(In general formula (D1), R ¹ to R ⁷ are each independently hydrogen or an organic group having 1 to 3 carbon atoms.)

In the above general formula (D1), R ¹ to R ⁷ are each independently hydrogen or an organic group having 1 to 3 carbon atoms, preferably hydrogen or an organic group having 1 carbon number, and hydrogen. It is even more preferable.
Further, the organic group constituting R ¹ to R ⁷ may contain atoms other than hydrogen and carbon in the structure of the organic group, for example.
Specifically, the organic groups constituting R ¹ to R ⁷ include alkyl groups such as methyl group, ethyl group, and n-propyl group; alkenyl groups such as allyl group and vinyl group; alkynyl groups such as ethynyl group; Examples thereof include alkylidene groups such as methylidene group and ethylidene group; cycloalkyl groups such as cyclopropyl group; and heterocyclic groups such as epoxy group and oxetanyl group.
Specific examples of atoms other than hydrogen and carbon include oxygen atoms, nitrogen atoms, sulfur atoms, phosphorus atoms, silicon atoms, fluorine atoms, and chlorine atoms. Atoms other than hydrogen and carbon may include one or more of the above specific examples.

The upper limit of the weight average molecular weight Mw of the indene resin (D) is, for example, preferably 4,000 or less, more preferably 2,000 or less, even more preferably 1,500 or less, and even more preferably 1,000 or less. Preferably, it is particularly preferably 800 or less. Thereby, the compatibility between the indene resin (D) and the epoxy resin (A) can be increased, and the indene resin (D) can be appropriately dispersed in the resin composition.
The lower limit of the weight average molecular weight Mw of the indene resin (D) is, for example, preferably 400 or more, more preferably 500 or more, even more preferably 550 or more, and 600 or more. is more preferable. Thereby, the indene resin (D) can be appropriately dispersed in the resin composition. Therefore, the indene resin (D) can appropriately suppress an increase in internal stress.

The upper limit of the number average molecular weight Mn of the indene resin (D) is, for example, preferably 2,000 or less, more preferably 1,500 or less, even more preferably 1,000 or less, and even more preferably 700 or less. Preferably, it is particularly preferably 600 or less. Thereby, the compatibility between the indene resin (D) and the epoxy resin (A) can be increased, and the indene resin (D) can be appropriately dispersed.
Further, the lower limit of the number average molecular weight Mn of the indene resin (D) is, for example, preferably 200 or more, more preferably 300 or more, even more preferably 350 or more, and 400 or more. is more preferable. Thereby, the indene resin (D) can be appropriately dispersed in the resin composition. Therefore, the indene resin (D) can appropriately suppress an increase in internal stress.

Further, from the viewpoint of making the physical properties of each molecular chain of the indene resin (D) uniform, the upper limit value of the polydispersity of the indene resin (D) according to the present embodiment is, for example, 2.50 or less, and 2. It is preferably .00 or less, more preferably 1.80 or less, and even more preferably 1.70 or less. Further, from the same viewpoint as the upper limit, the lower limit of the polydispersity of the copolymer can be, for example, 1.00 or more, or 1.10 or more.
Note that polydispersity is expressed by weight average molecular weight Mw/number average molecular weight Mn, and means a degree of dispersion that indicates the width of molecular weight distribution.

The weight average molecular weight Mw, number average molecular weight Mn, and polydispersity Mw/Mn can be evaluated and calculated using, for example, polystyrene equivalent values obtained from a standard polystyrene (PS) calibration curve obtained by GPC measurement.

The measurement conditions for GPC measurement are, for example, as follows.
Tosoh gel permeation chromatography device HLC-8320GPC
Column: TSK-GEL Supermultipore HZ-M manufactured by Tosoh Corporation
Detector: RI detector for liquid chromatogram Measurement temperature: 40°C
Solvent: THF
Sample concentration: 2.0mg/ml

Specifically, the indene resin (D) containing the structural unit represented by the above general formula (D1) is an indene homooligomer or an indene homopolymer having the structural unit shown by the above general formula (D1) as a repeating unit. Can be mentioned.

In addition, the indene resin (D) of this embodiment may have a structural unit represented by the above general formula (D1) and a structural unit derived from another monomer other than the above as repeating units. It may also be a so-called indene co-oligomer or indene copolymer.
Specific examples of structural units derived from other monomers include those derived from monomers such as phenolic monomers, styrene monomers, coumaron monomers, and benzothiophene monomers, which will be detailed later.

In this embodiment, the indene resin (D) is preferably an indene copolymer or an indene co-oligomer, and more preferably an indene co-oligomer. Thereby, the indene resin (D) can be appropriately dispersed in the resin composition.

In addition, in this embodiment, an oligomer means a thing with a number average molecular weight of less than 10,000, and a polymer means a thing with a number average molecular weight of 10,000 or more.

When the indene resin (D) is an indene copolymer or an indene co-oligomer, the lower limit of the molar content of the structural unit represented by the general formula (D1) in the indene resin (D) is, for example, 50% or more. is preferable, more preferably 60% or more, even more preferably 70% or more, even more preferably 80% or more, and even more preferably 90% or more. Thereby, the mechanical strength of the cured product of the resin composition can be improved. Furthermore, it is possible to suppress an increase in internal stress when the resin composition is stored at high temperatures.
Further, when the indene resin (D) is an indene copolymer or an indene co-oligomer, the upper limit of the molar content of the structural unit represented by the general formula (D1) in the indene resin (D) is, for example, 99.5%. It can be as follows. Thereby, structural units other than the structural unit represented by general formula (D1) can improve the compatibility with the epoxy resin (A). Therefore, the dispersion state can be made appropriate, and an increase in internal stress when the resin composition is stored at high temperatures can be suppressed.

Next, the structural units derived from the other monomers mentioned above will be explained in detail.
Specific examples of the structural unit derived from a phenolic monomer include those represented by the following general formula (M1). Specific examples of the structural unit derived from a styrene monomer include those represented by the following general formula (M2). Specific examples of the structural unit derived from the coumaron-based monomer include those represented by the following general formula (M3). Specific examples of the structural unit derived from a benzothiophene monomer include those represented by the following general formula (M4).

(In general formula (M1), R ^P is hydrogen or an organic group having 1 to 3 carbon atoms. R ^P may be the same or different from each other.)

(In general formula (M2), R ^S is hydrogen or an organic group having 1 to 3 carbon atoms. R ^S may be the same or different from each other.)

(In general formula (M3), R ^C is hydrogen or an organic group having 1 to 3 carbon atoms. R ^C may be the same or different from each other.)

(In general formula (M4), R ^B is hydrogen or an organic group having 1 to 3 carbon atoms. R ^B may be the same or different from each other.)

In the above general formulas (M1) to (M4), R ^P , R ^S , R ^C and R ^B may each independently contain, for example, an atom other than hydrogen and carbon in the structure of the organic group.
Specific examples of atoms other than hydrogen and carbon include oxygen atoms, nitrogen atoms, sulfur atoms, phosphorus atoms, silicon atoms, fluorine atoms, and chlorine atoms. Atoms other than hydrogen and carbon may include one or more of the above specific examples.

In the above general formulas (M1) to (M4), R ^P , R ^S , R ^C and R ^B each independently represent, for example, hydrogen or an organic group having 1 to 3 carbon atoms; is preferably an organic group, and more preferably hydrogen.

In the above general formulas (M1) to (M4), the organic groups constituting R ^P , R ^S , R ^C and R ^B include alkyl groups such as methyl group, ethyl group, n-propyl group, etc. alkenyl groups such as allyl group and vinyl group; alkynyl groups such as ethynyl group; alkylidene groups such as methylidene group and ethylidene group; cycloalkyl groups such as cyclopropyl group; heterocyclic groups such as epoxy group and oxetanyl group. It will be done.

Among the above specific examples, the indene resin (D) preferably contains a structural unit derived from a phenolic monomer or a structural unit derived from a styrene monomer, and the indene resin (D) preferably contains a structural unit derived from a phenolic monomer and a structural unit derived from a styrene monomer. It is more preferable that the structural unit contains a structural unit.
Thereby, the compatibility between the epoxy resin (A) and the indene resin (D) can be further improved. Therefore, it is presumed that a more dispersed phase of the indene resin (D) can be formed, and an increase in the tensile modulus when the resin composition is stored at high temperatures can be suppressed.

For example, the lower limit of the content of the indene resin (D) is preferably 4 parts by mass or more, more preferably 7 parts by mass or more, and 10 parts by mass, based on 100 parts by mass of the epoxy resin (A). It is more preferably at least 12 parts by mass, even more preferably at least 12 parts by mass, and even more preferably at least 14 parts by mass. This makes it possible to suppress an increase in internal stress when the resin composition is stored at high temperatures.
The upper limit of the content of the indene resin (D) is, for example, preferably 50 parts by mass or less, more preferably 45 parts by mass or less, and 40 parts by mass, based on 100 parts by mass of the epoxy resin (A). It is more preferably at most 38 parts by mass, even more preferably at most 38 parts by mass. Thereby, the tensile modulus of the cured product of the resin composition after post-curing can be maintained appropriately.

The content of the indene resin (D) is preferably 0.1% by mass or more and 20% by mass or less, more preferably 0.2% by mass or more and 10% by mass or less, and Preferably it is 0.5% by mass or more and 8% by mass or less.
By setting the content of the indene resin (D) to the above lower limit value or more, the dielectric loss tangent can be lowered while maintaining good mechanical properties, and the fluidity can be improved. On the other hand, by controlling the content of the indene resin (D) to be less than or equal to the above upper limit, mechanical strength can be increased while maintaining a good low dielectric loss tangent.

The resin composition of this embodiment may further contain the following components.

[Coupling agent (E)]
The coupling agent (E) can suppress aggregation of the high dielectric constant filler (C) and any inorganic filler described below, and can provide good fluidity of the resin composition.
Examples of the coupling agent (E) include known coupling agents such as various silane compounds such as epoxysilane, mercaptosilane, aminosilane, alkylsilane, ureidosilane, and vinylsilane, titanium compounds, aluminum chelates, and aluminum/zirconium compounds. A ring agent can be used.

More specifically, vinyltrichlorosilane, vinyltrimethoxysilane, vinyltriethoxysilane, vinyltris(β-methoxyethoxy)silane, γ-methacryloxypropyltrimethoxysilane, β-(3,4-epoxycyclohexyl)ethyltri Methoxysilane, γ-glycidoxypropyltrimethoxysilane, γ-glycidoxypropyltriethoxysilane, γ-glycidoxypropylmethyldimethoxysilane, γ-methacryloxypropylmethyldiethoxysilane, γ-methacryloxypropyltriethoxy Silane, vinyltriacetoxysilane, γ-mercaptopropyltrimethoxysilane, γ-aminopropyltriethoxysilane, γ-anilinopropyltrimethoxysilane, γ-anilinopropylmethyldimethoxysilane, γ-[bis(β-hydroxyethyl )] Aminopropyltriethoxysilane, N-β-(aminoethyl)-γ-aminopropyltrimethoxysilane, N-β-(aminoethyl)-γ-aminopropyltriethoxysilane, N-β-(aminoethyl) -γ-aminopropylmethyldimethoxysilane, N-phenyl-γ-aminopropyltrimethoxysilane, γ-(β-aminoethyl)aminopropyldimethoxymethylsilane, N-(trimethoxysilylpropyl)ethylenediamine, N-(dimethoxymethyl) silylisopropyl) ethylenediamine, methyltrimethoxysilane, dimethyldimethoxysilane, methyltriethoxysilane, N-β-(N-vinylbenzylaminoethyl)-γ-aminopropyltrimethoxysilane, γ-chloropropyltrimethoxysilane, hexamethyl Disilane, vinyltrimethoxysilane, γ-mercaptopropylmethyldimethoxysilane, 3-isocyanatepropyltriethoxysilane, 3-acryloxypropyltrimethoxysilane, 3-triethoxysilyl-N-(1,3-dimethyl-butylidene) Silane coupling agents such as propylamine hydrolysates; isopropyl triisostearoyl titanate, isopropyl tris(dioctylpyrophosphate) titanate, isopropyl tri(N-aminoethyl-aminoethyl) titanate, tetraoctyl bis(ditridecyl phosphite) ) titanate, tetra(2,2-diallyloxymethyl-1-butyl)bis(ditridecyl)phosphite titanate, bis(dioctylpyrophosphate)oxyacetate titanate, bis(dioctylpyrophosphate)ethylene titanate, isopropyltrioctanoyltitanate, Titanate couplings such as isopropyl dimethacrylylisostearoyl titanate, isopropyl tridodecylbenzenesulfonyl titanate, isopropyl isostearoyl diacryl titanate, isopropyl tri(dioctyl phosphate) titanate, isopropyl tricumylphenyl titanate, tetraisopropyl bis(dioctyl phosphite) titanate, etc. Examples include agents. These may be used alone or in combination of two or more.
Among these, silane coupling agents are preferred.

The content of the coupling agent (E) is not particularly limited, but it is preferably 0.05% by mass or more and 3% by mass or less, and 0.1% by mass or more and 2% by mass or less, based on the entire resin composition. It is more preferable that By setting the content of the coupling agent (E) to the above lower limit or more, it is possible to improve the dispersibility of the inorganic filler and the like in the resin composition. In addition, by controlling the content of the coupling agent (E) to be at most the above upper limit, the resin composition can have good fluidity and improve moldability.

[Curing catalyst (F)]
The resin composition of this embodiment can further contain a curing catalyst (F).
The curing catalyst (F) is sometimes called a curing accelerator or the like. The curing catalyst (F) is not particularly limited as long as it accelerates the curing reaction of the thermosetting resin such as the epoxy resin (A), and any known curing catalyst can be used.

Specifically, phosphorus atom-containing compounds such as organic phosphines, tetra-substituted phosphonium compounds, phosphobetaine compounds, adducts of phosphine compounds and quinone compounds, and adducts of phosphonium compounds and silane compounds; 2-methylimidazole, 2- Imidazole such as phenylimidazole (imidazole curing accelerator); 1,8-diazabicyclo[5.4.0]undecene-7, benzyldimethylamine, etc. are examples of amidine and tertiary amine; quaternary of amidine and amine; Examples include nitrogen atom-containing compounds such as salts, and only one type or two or more types may be used.

Among these, from the viewpoint of improving hardenability and obtaining a magnetic material with excellent mechanical strength such as bending strength, it is preferable to include compounds containing phosphorus atoms, such as tetra-substituted phosphonium compounds, phosphobetaine compounds, phosphine compounds and quinone compounds. It is more preferable to include compounds with latent properties such as adducts between phosphonium compounds and silane compounds, tetra-substituted phosphonium compounds, adducts between phosphine compounds and quinone compounds, and adducts between phosphonium compounds and silane compounds. Adducts are particularly preferred.

In particular, by using the active ester curing agent (b1) represented by the above-mentioned general formula (1) in combination with a curing catalyst having latent properties, it is possible to obtain excellent moldability and mechanical strength such as bending strength. It is possible to obtain a magnetic material.

Examples of the organic phosphine include primary phosphines such as ethylphosphine and phenylphosphine; secondary phosphines such as dimethylphosphine and diphenylphosphine; and tertiary phosphines such as trimethylphosphine, triethylphosphine, tributylphosphine and triphenylphosphine.
Examples of the tetra-substituted phosphonium compound include compounds represented by the following general formula (6).

In general formula (6), P represents a phosphorus atom. R ⁴ , R ⁵ , R ⁶ and R ⁷ each independently represent an aromatic group or an alkyl group. A represents an anion of an aromatic organic acid having at least one functional group selected from a hydroxyl group, a carboxyl group, and a thiol group in its aromatic ring. AH represents an aromatic organic acid having at least one functional group selected from a hydroxyl group, a carboxyl group, and a thiol group in an aromatic ring. x and y are each from 1 to 3, z is from 0 to 3, and x=y.

The compound represented by general formula (6) can be obtained, for example, as follows.
First, a tetra-substituted phosphonium halide, an aromatic organic acid, and a base are mixed uniformly in an organic solvent, and an aromatic organic acid anion is generated in the solution system. Then, by adding water, the compound represented by general formula (6) can be precipitated.
In the compound represented by general formula (6), R ⁴ , R ⁵ , R ⁶ and R ⁷ bonded to the phosphorus atom are phenyl groups, and AH is a compound having a hydroxyl group in the aromatic ring, that is, a phenol. , and A is preferably an anion of the phenol. The above-mentioned phenols include monocyclic phenols such as phenol, cresol, resorcinol, and catechol; condensed polycyclic phenols such as naphthol, dihydroxynaphthalene, and anthraquinol; and bisphenols such as bisphenol A, bisphenol F, and bisphenol S; Examples include polycyclic phenols such as phenylphenol and biphenol.

Examples of the phosphobetaine compound include a compound represented by the following general formula (7).

In general formula (7), P represents a phosphorus atom. R ⁸ represents an alkyl group having 1 to 3 carbon atoms, and R ⁹ represents a hydroxyl group. f is 0-5 and g is 0-3.

The compound represented by general formula (7) can be obtained, for example, as follows.
First, a triaromatic substituted phosphine, which is a tertiary phosphine, is brought into contact with a diazonium salt, and the diazonium group of the triaromatic substituted phosphine and the diazonium salt is substituted.

Examples of the adduct of a phosphine compound and a quinone compound include a compound represented by the following general formula (8).

In general formula (8), P represents a phosphorus atom. R ¹⁰ , R ¹¹ and R ¹² each represent an alkyl group having 1 to 12 carbon atoms or an aryl group having 6 to 12 carbon atoms, and may be the same or different from each other. R ¹³ , R ¹⁴ and R ¹⁵ represent a hydrogen atom or a hydrocarbon group having 1 to 12 carbon atoms, and may be the same or different from each other, and R ¹⁴ and R ¹⁵ are bonded to form a cyclic structure. You can.

Examples of phosphine compounds used in the adduct of a phosphine compound and a quinone compound include triphenylphosphine, tris(alkylphenyl)phosphine, tris(alkoxyphenyl)phosphine, trinaphthylphosphine, tris(benzyl)phosphine, etc. It is preferable that the substituent is substituted or has a substituent such as an alkyl group or an alkoxyl group, and examples of the substituent such as an alkyl group or an alkoxyl group include those having 1 to 6 carbon atoms. Triphenylphosphine is preferred from the viewpoint of availability.

Furthermore, examples of the quinone compound used in the adduct of a phosphine compound and a quinone compound include benzoquinone and anthraquinones, and among them, p-benzoquinone is preferred from the viewpoint of storage stability.

As a method for producing an adduct of a phosphine compound and a quinone compound, the adduct can be obtained by contacting and mixing both the organic tertiary phosphine and the benzoquinone in a solvent that can dissolve them. The solvent is preferably a ketone such as acetone or methyl ethyl ketone, which has low solubility in the adduct. However, it is not limited to this.

In the compound represented by general formula (8), R ¹⁰ , R ¹¹ and R ¹² bonded to the phosphorus atom are phenyl groups, and R ¹³ , R ¹⁴ and R ¹⁵ are hydrogen atoms, that is, 1, A compound to which 4-benzoquinone and triphenylphosphine are added is preferred in that it lowers the thermal modulus of the cured product of the sealing resin composition.

Examples of the adduct of a phosphonium compound and a silane compound include a compound represented by the following general formula (9).

In general formula (9), P represents a phosphorus atom, and Si represents a silicon atom. R ¹⁶ , R ¹⁷ , R ¹⁸ and R ¹⁹ each represent an organic group having an aromatic ring or a heterocycle, or an aliphatic group, and may be the same or different from each other. R ²⁰ is an organic group bonded to groups Y ² and Y ³ . R ²¹ is an organic group bonded to groups Y ⁴ and Y ⁵ . Y ² and Y ³ represent a group formed by a proton-donating group releasing a proton, and the groups Y ² and Y ³ in the same molecule bond to a silicon atom to form a chelate structure. Y ⁴ and Y ⁵ represent a group formed by a proton-donating group releasing a proton, and the groups Y ⁴ and Y ⁵ in the same molecule bond to a silicon atom to form a chelate structure. R ²⁰ and R ²¹ may be the same or different from each other, and Y ² , Y ³ , Y ⁴ and Y ⁵ may be the same or different from each other. Z ¹ is an organic group having an aromatic ring or a heterocycle, or an aliphatic group.

In general formula (9), R ¹⁶ , R ¹⁷ , R ¹⁸ and R ¹⁹ are, for example, phenyl group, methylphenyl group, methoxyphenyl group, hydroxyphenyl group, naphthyl group, hydroxynaphthyl group, benzyl group, methyl group. , ethyl group, n-butyl group, n-octyl group, cyclohexyl group, etc. Among these, alkyl groups such as phenyl group, methylphenyl group, methoxyphenyl group, hydroxyphenyl group, hydroxynaphthyl group, and alkoxy groups , an aromatic group having a substituent such as a hydroxyl group, or an unsubstituted aromatic group is more preferable.

In general formula (9), R ²⁰ is an organic group bonded to Y ² and Y ³ . Similarly, R ²¹ is an organic group that is bonded to groups Y ⁴ and Y ⁵ . Y ² and Y ³ are groups formed by a proton-donating group releasing protons, and the groups Y ² and Y ³ in the same molecule bond to a silicon atom to form a chelate structure. Similarly, Y ⁴ and Y ⁵ are groups formed by a proton-donating group releasing protons, and the groups Y ⁴ and Y ⁵ in the same molecule combine with a silicon atom to form a chelate structure. The groups R ²⁰ and R ²¹ may be the same or different from each other, and the groups Y ² , Y ³ , Y ⁴ and Y ⁵ may be the same or different from each other.

The groups represented by -Y ² -R ²⁰ -Y ³ - and Y ⁴ -R ²¹ -Y ⁵ - in general formula (9) are groups in which the proton donor releases two protons. As a proton donor, an organic acid having at least two carboxyl groups or hydroxyl groups in the molecule is preferable, and furthermore, an organic acid having at least two carboxyl groups or hydroxyl groups in the molecule constituting the aromatic ring is preferable. An aromatic compound having at least two hydroxyl groups is preferred, and an aromatic compound having at least two hydroxyl groups on adjacent carbons constituting an aromatic ring is more preferred, such as catechol, pyrogallol, 1,2-dihydroxynaphthalene, 2,3-dihydroxy Naphthalene, 2,2'-biphenol, 1,1'-bi-2-naphthol, salicylic acid, 1-hydroxy-2-naphthoic acid, 3-hydroxy-2-naphthoic acid, chloranilic acid, tannic acid, 2-hydroxybenzyl Examples include alcohol, 1,2-cyclohexanediol, 1,2-propanediol, and glycerin, but among these, catechol, 1,2-dihydroxynaphthalene, and 2,3-dihydroxynaphthalene are more preferred.

^Z1 in the general formula (9) represents an organic group or aliphatic group having an aromatic ring or a heterocycle, and specific examples thereof include a methyl group, an ethyl group, a propyl group, a butyl group, and a hexyl group. and aliphatic hydrocarbon groups such as octyl groups, aromatic hydrocarbon groups such as phenyl, benzyl, naphthyl, and biphenyl groups, glycidyloxy groups such as glycidyloxypropyl, mercaptopropyl, and aminopropyl groups, and mercapto Among these, methyl, ethyl, phenyl, naphthyl, and biphenyl groups are more preferable in terms of thermal stability. preferable.
A method for producing an adduct of a phosphonium compound and a silane compound is, for example, as follows.

A silane compound such as phenyltrimethoxysilane and a proton donor such as 2,3-dihydroxynaphthalene are added and dissolved in a flask containing methanol, and then a sodium methoxide-methanol solution is added dropwise while stirring at room temperature. Furthermore, when a previously prepared solution of a tetra-substituted phosphonium halide such as tetraphenylphosphonium bromide dissolved in methanol is added dropwise thereto under stirring at room temperature, crystals are precipitated. When the precipitated crystals are filtered, washed with water, and dried under vacuum, an adduct of a phosphonium compound and a silane compound is obtained.

When using the curing catalyst (F), its content is preferably 0.1 to 10% by mass, more preferably 0.2 to 5% by mass, based on the entire resin composition. By setting the value within such a numerical range, a sufficient curing accelerating effect can be obtained without excessively deteriorating other performances.

[Inorganic filler]
The resin composition of the present embodiment can further contain an inorganic filler in addition to the high dielectric constant filler (C) in order to reduce hygroscopicity, reduce linear expansion coefficient, improve thermal conductivity, and improve strength.

Inorganic fillers include fused silica, crystalline silica, alumina, calcium silicate, calcium carbonate, potassium titanate, silicon carbide, silicon nitride, aluminum nitride, boron nitride, beryllia, zirconia, zircon, forsterite, steatite, spinel, Examples include powders such as mullite and titania, beads made of spherical powders, and glass fibers. These inorganic fillers may be used alone or in combination of two or more.
Among the above inorganic fillers, fused silica is preferred from the viewpoint of reducing the linear expansion coefficient, alumina is preferred from the viewpoint of high thermal conductivity, and the filler shape is spherical from the viewpoint of fluidity during molding and mold abrasion resistance. is preferred.

The content of the inorganic filler other than the high dielectric constant filler (C) is preferably 10% by mass or more and 30% by mass based on the entire resin composition from the viewpoint of moldability, reduction of thermal expansion, and improvement of strength. % or less, more preferably 12% by mass or more and 20% by mass or less. Within the above range, thermal expansion property reduction and moldability are excellent.

Next, the physical properties of the resin composition of this embodiment will be explained.

[Permittivity, dielectric loss tangent]
The resin composition of the present embodiment is prebaked at 120° C. for 4 minutes and heated at 200° C. for 90 minutes, and the dielectric constant (Dk: εr) at 1 MHz of the cured product is preferably 10 to 30. More preferably 12-25, still more preferably 15-20.
Further, the resin composition of the present embodiment is prebaked at 120°C for 4 minutes and heated at 200°C for 90 minutes, and the dielectric loss tangent (Df: tan δ) at 1 MHz of the cured product is preferably 0.0020 to 0.0020. 0.0050, more preferably 0.0020 to 0.0035, still more preferably 0.0020 to 0.0029.

[Mechanical properties]
(bending modulus)
The resin composition of the present embodiment has a flexural modulus of elasticity at 260°C measured by the following procedure, which is preferably 50 N/mm ² MPa or more, more preferably 55 N/mm ² MPa or more, and even more preferably is 60 N/mm ² MPa or more.
On the other hand, the bending elastic modulus at 260° C. is preferably 200 N/mm ² MPa or less, more preferably 150 N/mm ² MPa or less, even more preferably 110 N/mm ² or less. Thereby, good moldability of the resin composition can be maintained.

(Procedure) The molding resin composition was injected into a mold at a mold temperature of 130°C, an injection pressure of 9.8 MPa, and a curing time of 300 seconds, and then post-cured at 175°C for 4 hours. Prepare a test piece. Using the test piece, the flexural modulus is measured in accordance with JIS K 6911.

Further, the ratio of the bending strength at 260°C to the bending strength at room temperature (25°C) measured by the above procedure is preferably 0.001 to 0.009, more preferably 0.002 to 0. It is .006.
As a result, the temperature dependence of the mechanical strength of a molded article using the resin composition of this embodiment can be reduced, and more stable mechanical strength can be obtained.

(bending strength)
Further, the bending strength at 260°C measured by the above procedure is preferably 0.5 N/mm ² MPa or more, more preferably 1.0 N/mm ² MPa or more, and still more preferably 1.5 N/mm 2 MPa or more. /mm ² MPa or more.
On the other hand, the bending strength when bent at 260° C. is preferably 20 N/mm ² MPa or less, more preferably 10 N/mm ² MPa or less, and still more preferably 5 N/mm ² or less. Thereby, good moldability of the resin composition can be maintained.

[Gel time]
The resin composition of the present embodiment preferably has a gel time at 175° C. of 30 to 100 seconds, more preferably 40 to 80 seconds, and even more preferably 45 to 70 seconds.

[Spiral flow]
The resin composition of this embodiment has a spiral flow of 80 to 200 cm when the flow length (cm) is measured under the conditions of a mold temperature of 175°C, an injection pressure of 6.9 MPa, and a curing time of 120 seconds. The length is preferably 90 to 180 cm, more preferably 100 to 150 cm.

The resin composition of the present embodiment that satisfies the above characteristics can be obtained by appropriately selecting and combining an epoxy resin (A), a curing agent (B), a high dielectric constant filler (C), and an indene resin (D). It can be obtained by adjusting the ratio, etc. For example, the higher the content of the high dielectric constant filler (C), which has a higher dielectric constant, the easier it is to improve the dielectric constant. Further, for example, the higher the content of the indene resin (D), the easier it is to lower the dielectric loss tangent.

[Production method]
The thermosetting resin composition of this embodiment can be manufactured by uniformly mixing the above-mentioned components. Examples of the manufacturing method include a method in which a predetermined amount of raw materials is sufficiently mixed using a mixer, etc., then melt-kneaded using a mixing roll, kneader, extruder, etc., and then cooled and pulverized. The obtained thermosetting resin composition may be made into tablets with a size and mass suitable for molding conditions, if necessary.

<Cured product/molded product>
The cured product of this embodiment is obtained by thermally curing the above-mentioned molding resin composition at 165 to 185° C. for 90 to 180 seconds.
The molded article of the resin composition of the embodiment is formed by a molding method such as injection molding, metal in-mold molding, outsert molding, blow molding, extrusion molding, sheet molding, hot press molding, rotational molding, or laminated molding. This allows it to be processed into the desired molded product.

The cured product/molded product of this embodiment has a high dielectric constant and low dielectric loss tangent in a high frequency band, so it can be used for high frequencies, shortened circuits, and downsized communication equipment, etc., and can be used for microstrip antennas. It can be suitably used as a material for forming a dielectric waveguide, a material for forming an electromagnetic wave absorber, and the like.

<Microstrip antenna>
As shown in FIG. 1, the microstrip antenna 10 of this embodiment includes a dielectric substrate 12 formed by curing the above-mentioned thermosetting resin composition, and a radiation conductor provided on one surface of the dielectric substrate 12. It includes a plate (radiating element) 14 and a ground conductor plate 16 provided on the other surface of the dielectric substrate 12.

The shape of the radiation conductor plate may be rectangular or circular. In this embodiment, an example using a rectangular radiation conductor plate 14 will be explained.

The radiation conductor plate 14 includes any one of a metal material, an alloy of metal materials, a cured product of metal paste, and a conductive polymer. Metal materials include copper, silver, palladium, gold, platinum, aluminum, chromium, nickel, cadmium lead, selenium, manganese, tin, vanadium, lithium, cobalt, titanium, and the like. Alloys include multiple metallic materials. The metal paste agent includes one obtained by kneading a powder of a metal material with an organic solvent and a binder. The binder includes epoxy resin, polyester resin, polyimide resin, polyamideimide resin, and polyetherimide resin. Conductive polymers include polythiophene polymers, polyacetylene polymers, polyaniline polymers, polypyrrole polymers, and the like.

As shown in FIG. 1, the microstrip antenna 10 of this embodiment has a radiation conductor plate 14 with a length L and a width W, and resonates at a frequency where L corresponds to an integral multiple of 1/2 wavelength. . When using the dielectric substrate 12 having a high dielectric constant as in this embodiment, the thickness h of the dielectric substrate 12 and the width W of the radiation conductor plate 14 are designed to be sufficiently small with respect to the wavelength.

The ground conductor plate 16 is a thin plate made of a highly conductive metal such as copper, silver, or gold. The thickness may be sufficiently thin with respect to the center operating frequency of the antenna device, and may be about 1/50th to 1/1000th wavelength of the center operating frequency.

Power feeding methods for microstrip antennas include direct feeding methods such as back coaxial feeding and coplanar feeding, and electromagnetic coupling feeding methods such as slot coupled feeding and proximity coupled feeding.

In the rear coaxial power feeding, power can be fed from the back surface of the antenna to the radiation conductor plate 14 using a coaxial line or a connector that penetrates the ground conductor plate 16 and the dielectric substrate 12.
In coplanar power feeding, power can be fed to the radiation conductor plate 14 using a microstrip line (not shown) arranged on the same plane as the radiation conductor plate 14.

In the slot coupled power supply, another dielectric substrate (not shown) is provided to sandwich the ground conductor plate 16, and the radiation conductor plate 14 and the microstrip line are formed on separate dielectric substrates. The radiation conductor plate 14 is excited by electromagnetically coupling the radiation conductor plate 14 and the microstrip line through the slots formed in the ground conductor plate 16.

In the close-coupled power supply, the dielectric substrate 12 has a laminated structure, and includes a dielectric substrate on which the radiation conductor plate 14 is formed, and a dielectric substrate on which the strip conductor of the microstrip line and the ground conductor plate 16 are arranged. It is layered. The radiation conductor plate 14 is excited by extending the strip conductor of the microstrip line below the radiation conductor plate 14 and electromagnetically coupling the radiation conductor plate 14 and the microstrip line.

<Dielectric waveguide>
In this embodiment, the dielectric waveguide includes a dielectric formed by curing the thermosetting resin composition of this embodiment, and a conductive film covering the surface of the dielectric. A dielectric waveguide confines electromagnetic waves in a dielectric (dielectric medium) and transmits them.
The conductor film can be made of metal such as copper, oxide high temperature superconductor, or the like.

<Electromagnetic wave absorber>
In this embodiment, the electromagnetic wave absorber has a structure in which a support, a resistive film, a dielectric layer, and a reflective layer are laminated. The electromagnetic wave absorber can be used as a λ/4 type radio wave absorber having high radio wave absorption performance.
Examples of the support include resin base materials. The support can protect the resistive film and improve its durability as a radio wave absorber.
Examples of the resistive film include indium tin oxide and molybdenum-containing resistive films.
The dielectric layer is formed by curing the thermosetting resin composition of this embodiment. Its thickness is about 10 μm or more and 2000 μm or less.
The reflective layer can function as a radio wave reflective layer, and includes, for example, a metal film.

Although the embodiments of the present invention have been described above, these are merely examples of the present invention, and various configurations other than those described above can be adopted within a range that does not impair the effects of the present invention.

EXAMPLES The present invention will be explained in more detail with reference to Examples below, but the present invention is not limited thereto.

(1) Preparation of resin composition The following raw materials were mixed in the amounts shown in Table 1 using a mixer at room temperature, and then kneaded with rolls at 70 to 100°C. Next, the obtained kneaded product was cooled and then ground to obtain a powdery resin composition. Then, a tablet-shaped resin composition was obtained by compression molding under high pressure.

[material]
Epoxy resin (A)
・Epoxy resin 1: Biphenylene skeleton-containing phenol aralkyl epoxy resin (NC3000L, manufactured by Nippon Kayaku Co., Ltd.)

Hardening agent (B)
・Curing agent 1: Active ester curing agent synthesized by the following method (synthesis method of active ester curing agent)
203.0 g of 1,3-benzenedicarboxylic acid dichloride (number of moles of acid chloride group: 2.0 moles) and 1338 g of toluene were placed in a flask equipped with a thermometer, dropping funnel, cooling tube, fractionating tube, and stirrer. After charging, the system was replaced with nitrogen under reduced pressure to dissolve. Next, 96.5 g (0.67 mol) of α-naphthol and 219.5 g (mol number of phenolic hydroxyl group: 1.33 mol) of dicyclopentadiene phenol resin were charged, and the system was replaced with nitrogen under reduced pressure to dissolve them. Ta. Thereafter, while performing a nitrogen gas purge, the inside of the system was controlled at 60° C. or lower, and 400 g of a 20% aqueous sodium hydroxide solution was added dropwise over a period of 3 hours. Stirring was then continued under these conditions for 1.0 hour. After the reaction was completed, the mixture was allowed to stand still for liquid separation, and the aqueous layer was removed. Furthermore, water was added to the toluene phase in which the reactants were dissolved, and the mixture was stirred and mixed for about 15 minutes, and the mixture was allowed to stand still for liquid separation to remove the aqueous layer. This operation was repeated until the pH of the aqueous layer reached 7. Thereafter, water was removed by dehydration using a decanter to obtain an active ester resin in the form of a toluene solution with a nonvolatile content of 65%.
When the structure of the obtained active ester resin was confirmed, it had a structure in which R ¹ and R ³ are hydrogen atoms, Z is a naphthyl group, and l is 0 in the above formula (1-3). The average value k of the repeating units of the active ester resin was calculated from the reaction equivalence ratio and was in the range of 0.5 to 1.0.

High dielectric constant filler (C)
・High dielectric constant filler 1: Calcium titanate (average particle size 2.0 μm, dielectric constant 135)

Indene resin (D)
- Indene resin 1: indene-styrene-phenol cooligomer represented by the following formula (P) (molar content of indene-derived structural units from 90% to 99%, IP-100, weight average molecular weight Mw = 710, Number average molecular weight Mn = 420, polydispersity Mw/Mn = 1.69, manufactured by Nippon Steel Chemical & Materials)

Coupling agent (E)
・Coupling agent 1: Phenylaminopropyltrimethoxysilane (CF4083, manufactured by Dow Corning Toray)
・Coupling agent 2: 3-mercaptopropyltrimethoxysilane (Sila Ace, manufactured by JNC)

Curing catalyst (F)
・Catalyst 1: Tetraphenylphosphonium-4,4'-sulfonyl diphenolate

Others/Inorganic filler 1: Fused spherical silica (manufactured by Denka)
・Coloring agent 1: Black titanium oxide (Ako Kasei)
・Release agent 1: Glycerin trimontanate (Recolb WE-4, manufactured by Clariant Japan)

(2) Measurement/Evaluation The following measurements and evaluations were performed using the obtained resin composition. The results are shown in Table 1.

[Evaluation of permittivity and dielectric loss tangent by cavity resonator method]
First, a test piece was obtained using a resin composition according to the following procedure.
Each resin composition prepared in (1) above was applied to a Si substrate and prebaked at 120° C. for 4 minutes to form a resin film with a coating thickness of 12 μm. This was heated in an oven at 200° C. for 90 minutes under a nitrogen atmosphere, and treated with hydrofluoric acid (immersed in a 2% by mass hydrofluoric acid aqueous solution). After removing the substrate from the hydrofluoric acid, the cured film was peeled off from the Si substrate and used as a test piece.
The measurement devices used were a network analyzer HP8510C, a synthesized sweeper HP83651A, and a test set HP8517B (all manufactured by Agilent Technologies). These devices and a cylindrical cavity resonator (inner diameter 42 mm, height 30 mm) were set up.
The resonant frequency, 3 dB bandwidth, transmitted power ratio, etc. were measured at a frequency of 1 MHz with and without the test piece inserted into the resonator. Then, by analytically calculating these measurement results using software, dielectric properties such as permittivity (Dk) and dielectric loss tangent (Df) were determined. Note that the measurement mode was set to TE011 mode.

[Measurement of spiral flow (ST)]
Using a low-pressure transfer molding machine (KTS-15 manufactured by Kotaki Seiki Co., Ltd.), a mold for spiral flow measurement according to EMMI-1-66 was molded at a mold temperature of 175°C, an injection pressure of 6.9 MPa, and a curing time. Each resin composition prepared in (1) above was injected for 120 seconds, and the flow length (cm) was measured.

[Gel Time (GT)]
Each resin composition prepared in (1) above was melted on a hot plate heated to 175° C., and then the time (in seconds) until it hardened was measured while kneading it with a spatula.

[Evaluation of mechanical strength (bending strength/flexural modulus)]
Each resin composition prepared in (1) above was molded using a low-pressure transfer molding machine (KTS-30 manufactured by Kotaki Seiki Co., Ltd.) at a mold temperature of 130°C, an injection pressure of 9.8 MPa, and a curing time of 300 seconds. It was injected into a mold under the following conditions. As a result, molded products each having a width of 10 mm, a thickness of 4 mm, and a length of 80 mm were obtained.
Next, each of the obtained molded products was post-cured at 175° C. for 4 hours to provide test pieces for evaluation of mechanical strength.
For each test piece, the bending strength (N/mm ² ) and flexural modulus (N/mm ² ) at room temperature (25° C.) or 260° C. were measured in accordance with JIS K 6911.

10 Microstrip antenna 12 Dielectric substrate 14 Radiation conductor plate 16 Ground conductor plate

Claims (17)

A molding resin composition comprising an epoxy resin (A), a curing agent (B), a high dielectric constant filler (C), and an indene resin (D) having a structural unit represented by the following general formula (D1).

(In general formula (D1), R ¹ to R ⁷ each independently represent hydrogen or an organic group having 1 to 3 carbon atoms.) The molding resin composition according to claim 1 or 2,
The dielectric constant (Dk: εr) at 1 MHz of the cured product of the molding resin composition is 10 to 30, and the dielectric loss tangent (Df: tan δ) at 1 MHz of the cured product of the molding resin composition is 0.0020 to 0.0020. 0.0050, a molding resin composition. The molding resin composition according to claim 1 or 2,
A molding resin composition having a flexural modulus of elasticity at 260° C. of 50 N/mm ² MPa or more as measured by the following procedure.
(Procedure) The molding resin composition was injected into a mold at a mold temperature of 130°C, an injection pressure of 9.8 MPa, and a curing time of 300 seconds, and then post-cured at 175°C for 4 hours. Prepare a test piece. Using the test piece, the flexural modulus at 260°C is measured in accordance with JIS K 6911. The molding resin composition according to claim 1 or 2,
A resin composition for molding, wherein the content of the indene resin (D) is 4 parts by mass or more and 50 parts by mass or less, based on 100 parts by mass of the epoxy resin (A). The molding resin composition according to claim 1 or 2,
A molding resin composition, wherein the indene resin (D) has a weight average molecular weight Mw of 400 to 4,000. The molding resin composition according to claim 1 or 2,
A molding resin composition, wherein the molar content of the structural unit represented by the general formula (D1) in the indene resin (D) is 50% or more. The molding resin composition according to claim 1 or 2,
The high dielectric constant filler (C) is calcium titanate, barium titanate, strontium titanate, magnesium titanate, magnesium zirconate, strontium zirconate, bismuth titanate, zirconium titanate, zinc titanate, barium zirconate, A molding resin composition containing one or more selected from the group consisting of calcium zirconate titanate, lead zirconate titanate, barium magnesium niobate, and calcium zirconate. The molding resin composition according to claim 1 or 2,
A molding resin composition in which the content of the high dielectric constant filler (C) is 50 to 90% by mass based on the total amount of the molding resin composition. The molding resin composition according to claim 1 or 2,
A molding resin composition having a gel time of 30 to 100 seconds at 175°C. The molding resin composition according to claim 1 or 2,
The epoxy resin (A) is a bisphenol A type epoxy resin, a bisphenol F type epoxy resin, a biphenylaralkyl type epoxy resin, a naphthalene type epoxy resin, a dinaphthol aralkyl type epoxy resin, a dicyclopentadiene type epoxy resin, and a glycidylamine type epoxy resin. A molding resin composition containing one or more selected from resins. The molding resin composition according to claim 1 or 2,
A molding resin composition in which the curing agent (B) contains an active ester curing agent and/or a phenolic curing agent. The molding resin composition according to claim 1 or 2,
A molding resin composition further comprising a coupling agent (E). The molding resin composition according to claim 1 or 2,
A molding resin composition further comprising a curing catalyst (F). The molding resin composition according to claim 1 or 2,
A molding resin composition used as a material for forming antennas. A cured product of the molding resin composition according to claim 1 or 2. A dielectric substrate obtained by curing the molding resin composition according to claim 1 or 2. The dielectric substrate according to claim 16,
a radiation conductor plate provided on one surface of the dielectric substrate;
a ground conductor plate provided on the other surface of the dielectric substrate;
Microstrip antenna.

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