Composition

Abstract

This composition comprises: (A) a curable hydrocarbon resin; (C) a promoter which is a metal compound or a semimetal compound; and (D) a chelating agent having one or two oxygen atoms in one molecule, the composition being characterized in that the amount of the component (D) per mol of the component (C) contained in the composition is 2 mol or more.

Description

[Technical Field]

[0001] The present invention relates to a composition and a method for producing the same. [Background technology]

[0002] As communication frequencies move into the gigahertz range and higher, there is a growing need for insulating materials with low dielectric properties. This is because transmission loss is known to be approximately equal to the sum of dielectric loss, which is proportional to the dielectric loss tangent, and conductor loss. However, it is difficult to achieve sufficiently low dielectric constants and dielectric loss with existing materials such as epoxy resins. For this reason, new monomers, also known as LDMs (Low Dielectric Macromonomers), are being explored as raw materials.

[0003] For example, Patent Document 1 discloses, as a type of LDM, a curable composition containing a specific olefin-aromatic vinyl compound-aromatic polyene copolymer and a specific additive resin, which can further reduce the dielectric constant and dielectric loss.

[0004] As described in Patent Document 1, compounds containing metals or metalloids such as zirconium, hafnium, aluminum, boron, etc. are used as catalysts or promoters in the synthesis of LDM products, and such catalysts and promoters are usually not removed but remain in the final product.

[0005] On the other hand, it is known that the presence of aluminum residues in an olefin polymerization solution can cause fisheyes to form in the resulting film, and therefore, the addition of an aluminum trapping agent has been used to suppress the formation of fisheyes (Patent Document 2). [Prior art documents] [Patent documents]

[0006] [Patent Document 1] International Publication No. 2021 / 112088 [Patent Document 2] Japanese Patent Application Laid-Open No. 2000-001577 Summary of the Invention [Problem to be solved by the invention]

[0007] When conventional metal compounds are used as catalysts or co-catalysts in the production of LDM products, the resulting composition containing the catalyst residues can produce gel when exposed to the atmosphere. However, when conventional metal trapping agents are used to address this issue, the dielectric constant and dielectric loss are adversely affected.

[0008] Furthermore, the process of removing catalyst and co-catalyst residues is complicated, and there is also the problem that complete and reliable removal is difficult.

[0009] As a result, conventional technology has presented a new challenge in that it is difficult to prevent gel formation when manufacturing LDM products that require dielectric properties. [Means for solving the problem]

[0010] In order to solve the above problems, the present invention can provide the following aspects.

[0011] Aspect 1. (A) a curable hydrocarbon-based resin; (C) a cocatalyst which is a metal compound or a semimetal compound; (D) A chelating agent having one or two oxygen atoms in one molecule. A composition comprising: The amount of component (D) per 1 mol of component (C) contained in the composition is 2 mol or more. A composition characterized by:

[0012] Aspect 2. 2. The composition of embodiment 1, wherein the (A) component comprises an olefin-aromatic vinyl compound-aromatic polyene copolymer.

[0013] Aspect 3. The composition according to aspect 2, wherein the component (A) satisfies the following conditions (1) to (4): (1) The number average molecular weight of the copolymer is 500 or more and 100,000 or less. (2) The aromatic vinyl compound monomer unit is an aromatic vinyl compound having 8 to 20 carbon atoms, and the content of the aromatic vinyl compound monomer unit is 0 to 70% by mass. (3) The aromatic polyene monomer unit is one or more polyenes selected from polyenes having 5 to 20 carbon atoms and having a plurality of vinyl groups and / or vinylene groups in the molecule, and the content of vinyl groups and / or vinylene groups derived from the aromatic polyene monomer unit is 1.5 or more and less than 20 per number average molecular weight. (4) The olefin monomer unit is one or more olefins selected from olefins having 2 to 20 carbon atoms, and the total of the olefin monomer units, aromatic vinyl compound monomer units, and aromatic polyene monomer units is 100% by mass.

[0014] Aspect 4. (B) a resin component containing at least one selected from the group consisting of a thermoplastic hydrocarbon elastomer and a thermoplastic conjugated diene polymer; 4. The composition of any one of aspects 1 to 3, further comprising:

[0015] Aspect 5. Aspect 5: The composition according to any one of aspects 1 to 4, wherein the amount of component (D) is 0.5 parts by mass or more and 10 parts by mass or less, based on 100 parts by mass of component (A).

[0016] Aspect 6. (E) A catalyst that is a metal compound or a semimetal compound 6. The composition of any one of aspects 1 to 5, further comprising:

[0017] Aspect 7. The composition according to embodiment 6, wherein the amount of component (D) contained in the composition per 1 mole of component (E) is 100 mol or more.

[0018] Aspect 8. Aspect 8. The composition according to any one of aspects 1 to 7, wherein component (D) does not contain a nitrogen atom in the molecule.

[0019] Aspect 9. Aspect 9. The composition of any one of Aspects 1 to 8, wherein component (D) comprises one or more selected from the group consisting of 4-tert-butylcatechol and acetylacetone.

[0020] Aspect 10. A cured product of the composition according to any one of aspects 1 to 9.

[0021] Aspect 11. A laminate comprising a layer containing the composition according to any one of embodiments 1 to 9 and a metal foil.

[0022] Aspect 12. A single-layer CCL, multi-layer CCL, single-layer FCCL, or multi-layer FCCL substrate comprising the cured body of embodiment 10.

[0023] Aspect 13. A solution comprising the composition according to any one of aspects 1 to 9 and a solvent for dissolving the composition. [Effects of the Invention]

[0024] The composition according to the present invention has the effect of preventing gel generation during the manufacturing process of LDM products that require dielectric properties. DETAILED DESCRIPTION OF THE INVENTION

[0025] In this specification, the term "sheet" also encompasses the concept of a film. Furthermore, the term "film" as used herein also encompasses the concept of a sheet. In this specification, the term "composition" encompasses the concept of a varnish. That is, a liquid composition is referred to as a varnish. The order of the steps included in the method disclosed herein may be freely changed in chronological order as long as the effect can be achieved. Numerical ranges in this specification include the lower and upper limits unless otherwise specified.

[0026] The composition according to the present invention is characterized by containing a metal compound or semimetal compound as a promoter (C), and a chelating agent having one or two oxygen atoms per molecule (D), in a predetermined ratio. The amount of component (D) per mole of component (C) contained in the composition is 2 mol or more, preferably 2 mol to 10 mol, and more preferably 2 mol to 7 mol. If the amount of component (D) per mole of component (C) contained in the composition is less than 2 mol, problems such as gel formation when the composition is exposed to the atmosphere or an increase in viscosity when water is added can occur.

[0027] Component (C) is a co-catalyst that can be used in a catalytic amount in the polymerization of component (A), a curable hydrocarbon-based resin (hereinafter sometimes simply referred to as "resin") Component (C) may include, for example, one or more of any aluminum compounds or boron compounds.

[0028] Examples of aluminum compounds include organoaluminum compounds. Examples of organoaluminum compounds include methylaluminoxane (also called methylalumoxane or MAO), modified methylaluminoxane (also called modified MAO, MMAO), and solid polymethylaluminoxane (also called SMAO). These are commercially available from Tosoh Corporation under the trade names TMAO-312, TMAO-211, TMAO-212, MMAO-3A, ​​TMAO-341, and solid MAO. Further examples include alkylaluminum compounds such as triisobutylaluminum and triethylaluminum.

[0029] Examples of boron compounds include organic boron compounds, such as boronic acid, boronate ester, boron trifluoride alkyl ether, and boron trifluoride phenol.

[0030] Further examples of component (C) (and component (E) described below) may include those described in European Patent Application Publication No. 0872492A2, Japanese Patent Application Publication No. H11-130808, Japanese Patent Application Publication No. H9-309925, International Publication No. 00 / 20426, European Patent Application Publication No. 0985689A2, and Japanese Patent Application Publication No. H6-184179.

[0031] The amount of component (C) is preferably in the range of 0.01 to 10 parts by mass, and more preferably 0.1 to 1 part by mass, per 100 parts by mass of component (A). In this specification, when component (A) and component (B) are included, they may be collectively referred to as the "polymerization system."

[0032] Component (D) is a chelating agent having one or two oxygen atoms per molecule, and preferably does not contain a nitrogen atom. Three or more oxygen atoms per molecule can lead to problems such as poor dielectric properties in the cured product of the composition. Component (D) coordinates with and neutralizes the catalyst residue of component (C) after it has functioned as a catalyst or co-catalyst. Component (D) can also coordinate with and neutralize component (E), described below.

[0033] Without wishing to be bound by any particular theory, it is speculated that the chelating agent, having multiple groups containing oxygen atoms (preferably hydroxyl groups or carbonyl groups not containing nitrogen atoms), can efficiently coordinate with component (C) dissolved in the polymerization system and sufficiently detoxify it. It is also preferable that component (D) does not have an ester structure in its molecule.

[0034] The amount of component (D) is preferably at least 0.5 parts by weight, more preferably at least 0.6 parts by weight, more preferably at least 0.5 parts by weight or at least 0.6 parts by weight but not more than 10 parts by weight, and even more preferably at least 0.6 parts by weight but not more than 7 parts by weight, per 100 parts by weight of component (A). When the amount of component (D) is within the preferred range, catalyst residues can be sufficiently neutralized and the dielectric properties of the composition are less likely to be adversely affected. When the amount of component (D) is within the preferred range, the chelating agent is sufficiently dispersed throughout the resin component, which helps prevent gel formation when exposed to the atmosphere and also helps prevent thickening when water is added.

[0035] Component (A) may be any curable hydrocarbon resin having functional groups that can be thermally cured or cured in the presence of a radical polymerization initiator. The presence of component (A) allows the cured product of this composition to meet the heat resistance required for an electrical insulating material. The functional groups are not limited as long as they are thermally or radically curable, but are preferably one or more of the group consisting of vinyl, vinylene, and allyl groups. For example, component (A) may be a polyfunctional vinyl aromatic copolymer obtained by cationic polymerization, as described in International Publication Nos. 2018 / 181842 and 2017 / 115813; a polyphenylene ether resin having functional groups, such as SA-9000 from SABIC or OPE-2St from Mitsubishi Gas Chemical Company; a polyether (ketone) having functional groups; or a polymer or copolymer having a 1,2-polybutadiene structure, such as Cray Valley's "Ricon" brand. Further examples include olefin-aromatic vinyl compound-aromatic polyene copolymers obtained by single-site coordination polymerization. The component (A) may be a single component or a composition consisting of a plurality of components. Most preferably, the component (A) may comprise a polyfunctional vinyl aromatic copolymer or an olefin-aromatic vinyl compound-aromatic polyene copolymer, the constituents of which are essentially carbon atoms and hydrogen atoms.

[0036] A composition according to a preferred embodiment of the present invention contains an olefin-aromatic vinyl compound-aromatic polyene copolymer (hereinafter sometimes simply referred to as "copolymer") as component (A). The copolymer is characterized by being obtained by copolymerizing the olefin, aromatic vinyl compound, and aromatic polyene monomers through a single-site coordination polymerization reaction involving the participation of component (C).

[0037] The olefin monomer is at least one selected from α-olefins having from 2 to 20 carbon atoms and cyclic olefins having from 5 to 20 carbon atoms. These compounds are composed of carbon and hydrogen and are substantially free of oxygen, nitrogen, and halogens. Examples of α-olefins having from 2 to 20 carbon atoms include ethylene, propylene, 1-butene, 1-hexene, 1-octene, 1-decene, 1-dodecene, 4-methyl-1-pentene, and 3,5,5-trimethyl-1-hexene. Examples of cyclic olefins having from 5 to 20 carbon atoms include norbornene and cyclopentene. The olefin preferably used is a combination of ethylene with an α-olefin other than ethylene or a cyclic olefin, or ethylene alone. Ethylene alone, or a mass ratio of the α-olefin component other than ethylene contained therein to the ethylene component is preferably 1 / 7 or less, more preferably 1 / 10 or less, because this increases the peel strength of the resulting cured product with copper foil or copper wiring. More preferably, the content of α-olefin monomer components other than ethylene in the copolymer is 6% by mass or less, and even more preferably 4% by mass or less, or the olefin is ethylene alone. The glass transition temperature of the cured product of the copolymer described below can be adjusted by the type and content of the olefin.

[0038] When the total of the olefin monomer units, aromatic vinyl compound monomer units, and aromatic polyene monomer units is taken as 100% by mass, the content of the olefin monomer units in this copolymer may be preferably 20% by mass or more, more preferably 25% by mass or more, and most preferably 30% by mass or more. When the content of the olefin monomer units is 20% by mass or more, the toughness (elongation) and impact resistance of the final cured product are improved, and cracks during curing or during heat cycle testing of the cured product are less likely to occur. In this copolymer, the content of the olefin monomer units is preferably 90% by mass or less.

[0039] The aromatic vinyl compound monomer is an aromatic vinyl compound having 8 to 20 carbon atoms, and examples thereof include styrene, paramethylstyrene, paraisobutylstyrene, various vinylnaphthalenes, and various vinylanthracenes.

[0040] The content of aromatic vinyl compound monomer units in the copolymer may be 0% by mass or more and 70% by mass or less, preferably 10% by mass or more and 60% by mass or less. A content of aromatic vinyl compound monomer units of 70% by mass or less is preferable because the glass transition temperature of the cured product of the final resin composition is lower than near room temperature, improving toughness and elongation at low temperatures. A content of aromatic vinyl compound monomer units of 10% by mass or more improves the aromaticity of the copolymer, improving compatibility with flame retardants and fillers, preventing bleed-out of flame retardants, and improving filler loading. Furthermore, a content of aromatic vinyl compound monomer units of 10% by mass or more can also produce a cured product with high peel strength from copper foil or copper wiring.

[0041] The aromatic polyene monomer may be a polyene having 5 to 20 carbon atoms and containing multiple vinyl and / or vinylene groups in its molecule. Preferably, the aromatic polyene monomer is a compound having an aromatic vinyl structure, such as ortho-, meta-, or para-divinylbenzene or a mixture thereof, divinylnaphthalene, divinylanthracene, p-2-propenylstyrene, or p-3-butenylstyrene, and consisting essentially of carbon and hydrogen and substantially free of oxygen, nitrogen, or halogens. Also usable are bifunctional aromatic vinyl compounds, such as 1,2-bis(vinylphenyl)ethane (abbreviated as BVPE), as described in JP 2004-087639 A. Among these, ortho-, meta-, or para-divinylbenzene or a mixture thereof is preferred, with a mixture of meta- and para-divinylbenzene being most preferred. In this specification, these divinylbenzenes are sometimes collectively referred to as divinylbenzenes. Divinylbenzenes are preferred as aromatic polyenes because they provide high curing efficiency and are easy to cure during curing treatment.

[0042] The above-mentioned olefin, aromatic vinyl compound, and aromatic polyene monomers may also contain polar groups, such as olefins containing oxygen atoms, nitrogen atoms, etc., aromatic vinyl compounds containing oxygen atoms, nitrogen atoms, etc., or aromatic polyenes containing oxygen atoms, nitrogen atoms, etc. The total mass of these polar group-containing monomers is preferably 10 mass% or less of the total mass of the composition, more preferably 3 mass% or less, and most preferably no polar group-containing monomers are included. By keeping the total mass ratio of polar group-containing monomers at 10 mass% or less, the dielectric properties (low dielectric constant, low dielectric loss) of the cured body obtained by curing the composition can be improved.

[0043] Among the present copolymers, examples of embodiments that do not contain aromatic vinyl compound monomer units (olefin-aromatic polyene copolymers) include ethylene-divinylbenzene copolymer, ethylene-propylene-divinylbenzene copolymer, ethylene-1-butene-divinylbenzene copolymer, ethylene-1-hexene-divinylbenzene copolymer, and ethylene-1-octene-divinylbenzene copolymer.

[0044] Among the present copolymers, examples of embodiments containing aromatic vinyl compound monomer units (olefin-aromatic vinyl compound-aromatic polyene copolymers) include ethylene-styrene-divinylbenzene copolymer, ethylene-propylene-styrene-divinylbenzene copolymer, ethylene-1-hexene-styrene-divinylbenzene copolymer, ethylene-1-octene-styrene-divinylbenzene copolymer, etc.

[0045] The number average molecular weight (Mn) of the copolymer may be from 500 to 100,000, preferably from 500 to 50,000, further preferably from 500 to 20,000, and even more preferably from 500 to 10,000. When Mn is 100,000 or less, it becomes possible to obtain a viscosity appropriate for a varnish, and the effect of improving the handleability when using the composition is obtained.

[0046] The weight-average molecular weight (Mw) of the present copolymer may be preferably from 10,000 to 200,000, more preferably from 20,000 to 200,000, and even more preferably from 20,000 to 150,000. The value Mw / Mn obtained by dividing the weight-average molecular weight by the number-average molecular weight may preferably be in the range of 2.0≦Mw / Mn≦13.0, more preferably 2.0≦Mw / Mn≦12.0, and even more preferably 2.0≦Mw / Mn≦10.0.

[0047] The number-average molecular weight and weight-average molecular weight in this specification refer to values ​​measured as molecular weights converted into standard polystyrene by high-temperature gel permeation chromatography (HT-GPC). The measurement conditions for HT-GPC in this specification are as follows: Measuring equipment: Tosoh HLC-8321GPC / HT Column: TSKgelGMHHR-H(20)HT, φ7.8 x 300mm, 3 pcs Column temperature: 140℃ Detector: RI Solvent: orthodichlorobenzene Flow rate: 1.0 ml / min Sample concentration: 0.2 wt / vol% Sample injection volume: 100 μL

[0048] In this copolymer, the content of vinyl groups and / or vinylene groups (preferably vinyl groups) derived from aromatic polyene units may be 1.5 or more and less than 20, preferably 2 or more and less than 7, per number average molecular weight. When the content of vinyl groups and / or vinylene groups is 1.5 or more, crosslinking efficiency is high, and a cured product with sufficient crosslinking density can be obtained. The content of vinyl groups derived from aromatic polyene units (divinylbenzene units) per number average molecular weight in the copolymer can be calculated by the number average molecular weight (Mn) calculated in terms of standard polystyrene determined by GPC (gel permeation chromatography) known to those skilled in the art, and 1 This can be obtained by comparing the vinyl group content derived from aromatic polyene units obtained by H-NMR measurement. For example, 1 By comparing the intensity of each peak area obtained by H-NMR measurement, if the content of vinyl groups derived from aromatic polyene units (divinylbenzene units) in the copolymer is 3.2% by mass, and the number average molecular weight converted to standard polystyrene by GPC measurement is 2100, the molecular weight of vinyl groups derived from aromatic polyene units in the number average molecular weight is the product of these, 67.5, which is divided by the formula weight of the vinyl groups, 27, to obtain 2.5. In other words, the content of vinyl groups derived from aromatic polyene units per number average molecular weight in this copolymer is calculated to be 2.5. 1 The assignment of peaks obtained by H-NMR measurement is known from literature. 1 A method for determining the composition of a copolymer from a comparison of peak areas obtained by H-NMR measurement is also known. In this specification, the content of divinylbenzene units in a copolymer is determined based on the peak intensity ( 1 This is determined from the content of vinyl groups derived from divinylbenzene units (measured by H-NMR). In other words, the content of divinylbenzene units is determined from the content of vinyl groups derived from divinylbenzene units, assuming that one vinyl group is derived from one divinylbenzene unit in the copolymer.

[0049] <Curable polyether resin> Component (A) may contain a curable polyether-based resin such as a curable polyphenylene ether or polyether. Commercially available known polyphenylene ethers can be used as such polyphenylene ethers. The number-average molecular weight of the polyphenylene ether is optional. Considering the moldability of the composition, the number-average molecular weight is preferably 10,000 or less, and most preferably 5,000 or less. The number-average molecular weight is preferably 500 or more, and most preferably 1,000 or more. Furthermore, when added for the purpose of curing the present composition, it is preferable that the molecular end is modified and / or that one molecule contains multiple functional groups. Examples of functional groups include allyl, vinyl, and epoxy groups. Radical-polymerizable functional groups are most preferred, particularly vinyl groups, and even more preferably one or more of the group consisting of (meth)acrylic and aromatic vinyl groups. In other words, in the present composition, bifunctional polyphenylene ethers in which both molecular chain ends are modified with radical-polymerizable functional groups are particularly preferred. Examples of such polyphenylene ethers include Noryl (trademark) SA9000 manufactured by SABIC, and particularly preferably, bifunctional polyphenylene ether oligomer (OPE-2St) manufactured by Mitsubishi Gas Chemical Company, Inc. The amount of polyphenylene ether used in the composition is preferably 1 to 200 parts by mass, more preferably 10 to 100 parts by mass, per 100 parts by mass of the copolymer. Furthermore, aromatic polyethers (ELPAC HC-F series) manufactured by JSR Corporation and the like can also be used as polyether-based resins. The amount of polyphenylene ether or other polyether-based resins used in the composition is preferably 1 to 200 parts by mass, more preferably 1 to 100 parts by mass, per 100 parts by mass of component (A).

[0050] <Curable aromatic polyene resin> The curable aromatic polyene resin that may be contained in component (A) includes divinylbenzene-based reactive hyperbranched copolymer (PDV) manufactured by Nippon Steel Chemical & Material Co., Ltd. Such PDV is described, for example, in the literature "Synthesis of Polyfunctional Aromatic Vinyl Copolymer and Development of New IPN-Type Low Dielectric Loss Materials Using the Same" (Kawabe Masanao et al., Journal of the Japan Institute of Electronics Packaging, p. 125, Vol. 12 No. 2 (2009)). Further examples of aromatic polyene resins include aromatic polyene polymer resins whose main structural unit is the above-mentioned aromatic polyene monomer.

[0051] The composition may further contain, as component (B), a resin component containing at least one selected from the group consisting of a thermoplastic hydrocarbon elastomer and a thermoplastic conjugated diene polymer. Component (B) is distinct from component (A) by definition, and does not include component (A) within its definition.

[0052] <Thermoplastic hydrocarbon elastomer> The amount of thermoplastic hydrocarbon-based elastomer that may be contained in component (B) is preferably 1 to 500 parts by mass, more preferably 1 to 200 parts by mass, per 100 parts by mass of the copolymer. Suitable hydrocarbon-based elastomers include one or more elastomers selected from ethylene-based or propylene-based elastomers, conjugated diene-based polymers, block or random copolymers of aromatic vinyl compounds and conjugated dienes, and hydrogenated products thereof. The number-average molecular weight of the hydrocarbon-based elastomer is 1,000 or more, more preferably 2,000 or more, even more preferably 20,000 or more, and most preferably 30,000 or more. The number-average molecular weight of the hydrocarbon-based elastomer is preferably 80,000 or less, more preferably 60,000 or less.

[0053] Examples of ethylene-based elastomers that may be contained in component (B) include ethylene-α-olefin copolymers such as ethylene-octene copolymer and ethylene-1-hexene copolymer, EPR, and EPDM, and examples of propylene-based elastomers include atactic polypropylene, low stereoregular polypropylene, and propylene-α-olefin copolymers such as propylene-1-butene copolymer.

[0054] Examples of thermoplastic conjugated diene polymers that may be contained in component (B) include polybutadiene and 1,2-polybutadiene. Examples of aromatic vinyl compound-conjugated diene block or random copolymers and their hydrogenated products include SBS, SIS, SEBS, SEPS, SEEPS, and SEEBS. Suitable 1,2-polybutadiene is available, for example, as a product from JSR Corporation, and also from Nippon Soda Co., Ltd. under the product names B-1000, 2000, and 3000 of liquid polybutadiene. Another suitable copolymer containing a 1,2-polybutadiene structure is "Ricon 100" from TOTAL CRAY VALLEY. When the resin or resins selected from these hydrocarbon elastomers are liquid (with a viscosity of approximately 300,000 mPa·S or less), particularly at room temperature (25°C), the amount used is preferably 1 to 30 parts by mass, and particularly preferably 1 to 20 parts by mass, per 100 parts by mass of the copolymer, from the viewpoint of the handleability and moldability of the composition in an uncured state (handleability as a thermoplastic resin).

[0055] The present composition may further contain optional additional components such as those exemplified below, as long as the effects of the composition are not impaired.

[0056] <Curing agent> As a curing agent that can be used in the present composition, a known curing agent that can be used for the polymerization or curing of conventional aromatic polyenes or aromatic vinyl compounds may be used. Examples of such curing agents include radical polymerization initiators, cationic polymerization initiators, and anionic polymerization initiators, but preferably radical polymerization initiators can be used. Preferred are organic peroxides, azo-based polymerization initiators, etc., and can be freely selected depending on the application and conditions. A catalog listing organic peroxides can be found on the NOF Corporation website, for example It can be downloaded from https: / / www.nof.co.jp / business / chemical / chemical-product01. Organic peroxides are also listed in catalogs from Fujifilm Wako Pure Chemical Industries, Ltd. and Tokyo Chemical Industry Co., Ltd. Curing agents are available from these companies. Known photopolymerization initiators that utilize light, ultraviolet light, or radiation can also be used as curing agents. Examples of curing agents that utilize photopolymerization initiators include photoradical polymerization initiators, photocationic polymerization initiators, and photoanionic polymerization initiators. Such photopolymerization initiators are available, for example, from Tokyo Chemical Industry Co., Ltd. Furthermore, curing using radiation or electron beams themselves is also possible. It is also possible to perform crosslinking and curing by thermal polymerization of the raw materials contained in the composition without using a curing agent.

[0057] There are no particular restrictions on the amount of curing agent used, but generally, 0.01 to 10 parts by mass per 100 parts by mass of the composition is preferred. The composition preferably excludes the curing agent and solvent. When using a curing agent such as a peroxide or azo-based polymerization initiator, the curing process should be carried out at an appropriate temperature and time, taking into account its half-life. The conditions for this can be determined arbitrarily depending on the curing agent, but a temperature range of approximately 50°C to 200°C is generally appropriate.

[0058] <Monomer> The amount of monomer that may be included in the composition is optional, but is preferably 10 parts by mass or less per 100 parts by mass of copolymer. The composition may be substantially free of monomer. When the monomer content is 10 parts by mass or less, the uncured composition does not become viscous, facilitating molding and processing as a thermoplastic resin. Furthermore, when the content of volatile monomers is below a certain level, odor in the uncured state is not an issue. When a solvent is added to the composition to produce a varnish-like product, the monomer is lost as the solvent evaporates during use, resulting in a problem of a decrease in the effective monomer content. Furthermore, when the product is in the form of an uncured sheet, containing a certain amount of monomer or less reduces the change in the monomer content during storage. Monomers suitable for use in the composition preferably have a molecular weight of less than 1,000, more preferably less than 500. Monomers suitable for use in the composition of the present invention include aromatic vinyl compound monomers, aromatic polyene monomers, and / or polar monomers. The monomer is preferably a monomer that can be polymerized with a radical polymerization initiator, and more preferably one or more members of the group consisting of the aromatic vinyl compounds and aromatic polyenes. Also, BVPE (1,2-bis(vinylphenyl)ethane) described in JP 2003-212941 A can be suitably used. From the viewpoint of increasing the mechanical strength (elastic modulus) of the cured product at high temperatures, the aromatic polyene is preferably used in an amount of 1 to 30 parts by mass per 100 parts by mass of the copolymer. Furthermore, a relatively small amount of a polar monomer can be used to impart adhesion to other materials required as an insulating material or to improve crosslink density. Examples of the polar monomer include various maleimides, bismaleimides, maleic anhydride, glycidyl (meth)acrylate, triallyl isocyanurate, tri(meth)acrylic isocyanurate, and trimethylolpropane tri(meth)acrylate. Usable maleimides and bismaleimides are described in, for example, WO 2016 / 114287 and JP 2008-291227 A, and can be purchased from, for example, Daiwa Chemical Industry Co., Ltd. or Designer Molecules Inc. Of these maleimide group-containing compounds, bismaleimides are preferred from the viewpoints of solubility in organic solvents, high-frequency characteristics, high adhesion to conductors, moldability of prepregs, and the like.

[0059] The bismaleimides are preferably those represented by the following formula (B-1).

[0060] Formula (B-1) [ka]

[0061] In formula (B-1), R represents an alkylene group having 5 or more carbon atoms, and L represents a single bond or a divalent linking group. R and L may each independently have a substituent. The maleimide represented by formula (B-1) is preferably represented by the following formula (B-2).

[0062] Formula (B-2) [ka]

[0063] In formula (B-2), R' each independently represents an alkylene group having 5 or more carbon atoms which may have a substituent, A each independently represents an alkylene group having 5 or more carbon atoms which may have a substituent or a divalent group having an aromatic ring which may have a substituent, and n represents an integer of 1 to 10.

[0064] Examples of the maleimides represented by formula (B-2) include compounds represented by the following formula (B-3), in which n represents an integer of 1 to 10. Examples of the compound represented by formula (B-3) include BMI-1500 (average n value=1.3) manufactured by Designer Molecules Inc.

[0065] Formula (B-3) [ka]

[0066] Bismaleimides may be used as polyaminobismaleimide compounds. Polyaminobismaleimide compounds can be obtained, for example, by subjecting a compound having two maleimide groups at its terminals to a Michael addition reaction with an aromatic diamine compound having two primary amino groups in its molecule. To achieve high crosslinking efficiency with a small amount of addition, polar monomers having bifunctional or higher polyfunctional groups are preferred. Examples of such monomers include bismaleimides, triallyl isocyanurate (TAIC), and trimethylolpropane tri(meth)acrylate. The amount of polar monomer that may be contained in the composition is 0.1 to 10 parts by mass, preferably 0.1 to 5 parts by mass, per 100 parts by mass of the copolymer. Using 10 parts by mass or less can reduce the dielectric constant and dielectric loss tangent of the resulting cured product.

[0067] The composition may further include a catalyst (E), which is any metal or semimetallic compound that can be used in a catalytic amount in the polymerization of component (A). Component (E) is, by definition, distinct from and does not include component (C). Component (E) preferably includes one or more zirconium or hafnium compounds.

[0068] The zirconium compound or hafnium compound includes a compound represented by the following general formula (I). [ka] In the above formula, M is an element selected from zirconium or hafnium. Cp1 and Cp2 are cyclopentadienyl groups having no substituents, or cyclopentadienyl groups having one or two alkyl substituents (preferably having 1 to 3 carbon atoms) having no cyclic structure. Cp1 and Cp2 may be the same or different. One of the Cp1 and Cp2 groups may be an indenyl group having no substituents, or an indenyl group having one or two alkyl substituents (preferably having 1 to 3 carbon atoms) having no cyclic structure. Y is an element selected from carbon, silicon, germanium, or boron having a bond with Cp1 and Cp2 and a hydrogen atom or a substituent, and the substituents (preferably alkyl groups, phenyl groups, etc.) may be different or the same and may have a cyclic structure (cyclohexyl structure, etc.). Each X is independently selected from the group consisting of hydrogen, halogen, an alkyl group, and an aryl group, or two Xs combine to form a diene group.

[0069] Examples of such zirconium compounds or hafnium compounds include dimethylmethylenebiscyclopentadienylzirconium dichloride, diphenylmethylenebiscyclopentadienylzirconium dichloride, dimethylmethylene(cyclopentadienyl)(1-indenyl)zirconium dichloride, and diphenylmethylene(cyclopentadienyl)(1-indenyl)zirconium dichloride.

[0070] The amount of component (D) per mole of component (E) contained in the composition may be 100 mol or more, preferably 100 mol to 500 mol, and the amount of component (E) per 100 parts by mass of component (A) may be in the range of 0.001 to 10 parts by mass, more preferably 0.01 to 5 parts by mass.

[0071] <Solvent> An appropriate solvent may be added to the composition as needed. The solvent is used to adjust the viscosity and fluidity of the composition. Volatile solvents are preferred, such as cyclohexane, toluene, ethylbenzene, acetone, and isopropanol. The amount of solvent used is preferably 10 parts by mass or less per 100 parts by mass of copolymer, from the viewpoint of moldability and handling of the composition as a thermoplastic resin before curing. Furthermore, from the viewpoint of removal during and after curing, it is more preferable that substantially no solvent is used. "Substantially no solvent" preferably means 5 parts by mass or less, more preferably 1 part by mass or less, and most preferably 0 parts by mass. When used as a varnish, it is preferable to add an appropriate solvent to the composition. The solvent is used to adjust the viscosity and fluidity of the composition as a varnish. A solvent with a high boiling point at atmospheric pressure, i.e., low volatility, results in a uniform thickness of the applied film; therefore, a solvent with a boiling point above a certain level is preferred. A preferred boiling point is generally 100°C or higher at atmospheric pressure, preferably 130°C to 300°C. Suitable solvents for such varnishes include toluene, xylene, mesitylene, ethylbenzene, limonene, ethylene glycol methyl ether acetate, ethylene glycol monoethyl ether acetate, ethylene glycol monobutyl ether, etc. The amount of the solvent used is preferably in the range of 10 to 2000 parts by mass per 100 parts by mass of the composition.

[0072] The composition may further contain one or more selected from a filler, a flame retardant, and a surface modifier. The composition can serve as a matrix for a cured body. The composition may contain one or more selected from a filler, a flame retardant, and a surface modifier to improve the filling of other materials when cured, and by doing so, the cured body can easily exhibit impact resistance and toughness even after curing.

[0073] <Filler> The composition may contain inorganic or organic fillers. These fillers are added for the purposes of controlling the coefficient of thermal expansion, controlling thermal conductivity, and reducing cost, and the amount used can be arbitrary depending on the purpose. The composition can contain a particularly large amount of inorganic filler, with the usable amount reaching a maximum of 2,000 parts by mass per 100 parts by mass of copolymer. When adding an inorganic filler, it is preferable to use a known surface modifier, such as a silane coupling agent. In particular, for the purpose of achieving a composition with low dielectric constant and low dielectric loss, which is one of the objects of the present invention, boron nitride (BN) and / or silica are preferred as inorganic fillers, with silica being more preferred. Of the silicas, fused silica is preferred. From the perspective of low dielectric properties, adding a large amount of filler may result in a particularly high dielectric constant. Therefore, it is preferable to use less than 500 parts by mass, more preferably less than 400 parts by mass, of filler per 100 parts by mass of copolymer. Furthermore, in order to improve and enhance low dielectric properties (low dielectric constant, low dielectric loss tangent), hollow fillers or fillers with many voids may be added.

[0074] Instead of inorganic fillers, organic fillers such as high-molecular-weight or ultra-high-molecular-weight polyethylene can also be used. It is preferable that the organic filler itself is crosslinked from the viewpoint of heat resistance, and it is preferable to use it in the form of fine particles or powder. These organic fillers can suppress increases in the dielectric constant and dielectric loss tangent. The most preferable amount of filler used is 1 part by mass or more but less than 400 parts by mass per 100 parts by mass of the copolymer.

[0075] On the other hand, by mixing and dispersing a high-dielectric-constant insulating filler having a dielectric constant of preferably 3 to 10,000, more preferably 5 to 10,000 at 1 GHz, into the present composition, it is possible to produce a cured insulating product having a high-dielectric-constant insulating layer with a dielectric constant of preferably 3.1 to 20 while suppressing an increase in dielectric loss tangent (dielectric loss). Increasing the dielectric constant of a film made from the cured insulating product enables the miniaturization of circuits and the increase in capacitance of capacitors, contributing to the miniaturization of high-frequency electrical components. High-dielectric-constant, low-dielectric-loss-tangent insulating layers are suitable for applications such as capacitors, inductors for resonant circuits, filters, and antennas. Examples of high-dielectric-constant insulating fillers used in the present invention include inorganic fillers or metal particles that have been subjected to an insulating treatment. Specific examples include known high-dielectric-constant inorganic fillers such as barium titanate and strontium titanate. Other examples are specifically described in, for example, JP 2004-087639 A.

[0076] <Flame retardant> The flame retardant that may be contained in the composition is, from the viewpoint of maintaining a low dielectric constant and a low dielectric loss tangent, a known organic phosphorus-based flame retardant such as a phosphate ester or a condensate thereof, a known bromine-based flame retardant, or red phosphorus. Among the phosphate esters, a compound having multiple xylenyl groups in the molecule is particularly preferred from the viewpoint of flame retardancy and a low dielectric loss tangent.

[0077] In addition to the flame retardant, antimony compounds such as antimony trioxide, antimony tetroxide, antimony pentoxide, and sodium antimonate, or nitrogen-containing compounds such as melamine, triallyl-1,3,5-triazine-2,3,4-(1H,3H,5H)-trione, and 2,4,6-triaryloxy-1,3,5-triazine may be added as a flame retardant aid. The total amount of these flame retardants and flame retardant aids is usually preferably 1 to 100 parts by mass per 100 parts by mass of the composition. Furthermore, 30 to 200 parts by mass of the polyphenylene ether (PPE) resin, which has a low dielectric constant and excellent flame retardancy, may be added per 100 parts by mass of the flame retardant.

[0078] <Surface modifier> The present composition may further contain various surface modifiers for the purpose of improving adhesion to fillers, copper plates, and wiring. The amount of the surface modifier used per 100 parts by mass of the present composition other than the surface modifier is preferably 0.01 to 10 parts by mass, more preferably 0.1 to 5 parts by mass. Examples of the surface modifier include various silane coupling agents and titanate coupling agents. The various silane coupling agents and titanate coupling agents may be used singly or in combination.

[0079] The present composition can also be made into a viscous liquid varnish by adjusting its composition and blending ratio. For example, a sufficient amount of solvent and / or an appropriate amount of liquid monomer can be used to produce a varnish. When using the composition as a varnish, it is preferable to add an appropriate solvent to the present composition. The solvent is used to adjust the viscosity and flowability of the composition as a varnish. A solvent with a high boiling point at atmospheric pressure, i.e., low volatility, is advantageous in achieving a uniform thickness for the applied film, so a solvent with a boiling point above a certain level is preferred. A preferred boiling point at atmospheric pressure is generally 100°C or higher, preferably 110°C to 300°C. Examples of solvents suitable for such varnishes include xylene, mesitylene, ethylbenzene, limonene, ethylene glycol methyl ether acetate, ethylene glycol monoethyl ether acetate, and ethylene glycol monobutyl ether. The amount of solvent used is preferably in the range of 10 to 2000 parts by mass per 100 parts by mass of the present composition. A varnish-like composition can also be produced using a polymerization liquid containing the present copolymer obtained by polymerization. For example, the polymerization solution may be concentrated or residual monomers may be removed, and if necessary, solvents, other resin components, various additives, etc. may be added to adjust the component concentrations and solution viscosity, etc., to produce the polymer.

[0080] The varnish can be applied to or impregnated into a substrate, and the solvent can be removed by drying or the like to form an uncured or semi-cured molded article. Generally, this molded article is in the form of a sheet, film, or tape.

[0081] <Curing> The composition can be cured by a known method, taking into consideration the curing conditions (temperature, time, pressure) of the curing agent contained therein. When the curing agent used is a peroxide, the curing conditions can be determined by taking into consideration the half-life temperature and the like disclosed for each peroxide.

[0082] The composition can be used as various insulating materials for wiring, preferably for high-frequency signal wiring, such as coverlays, solder resists, build-up materials, interlayer insulating agents, bonding sheets, interlayer adhesives, and bump sheets for flip-chip bonders. It can also be used as an electrical insulating layer or adhesive layer for substrates such as single-layer or multilayer printed circuit boards, flexible printed circuit boards, CCL (copper clad laminate), and FCCL (flexible copper clad laminate) substrates.

[0083] <Viscosity> In this specification, the viscosity of the composition is determined in accordance with JIS Z 8803:2011 when prepared as a 50% by mass toluene solution. The viscosity of the composition at 25°C is measured at a shear rate of 1 s -1 The viscosity may be 100,000 cP or less, preferably 10,000 cP or less or 9,000 cP or less, further preferably 8,000 cP or less, and even more preferably 5,000 cP or less. The lower limit of the viscosity is not particularly limited, but may be, for example, 500 cP or more, preferably 1,000 cP or more. When the viscosity is in this range, the effect of improving the handleability of the varnish can be obtained.

[0084] <Manufacturing method> The composition containing the copolymer described above can be obtained by subjecting a raw material solution prepared by mixing the olefin monomer, aromatic vinyl compound monomer, and aromatic polyene monomer described above in an appropriate solvent to a single-site coordination polymerization reaction. In another embodiment, a step of polymerizing in liquid monomer without using a solvent may be employed instead.

[0085] Usable solvents include saturated aliphatic or aromatic hydrocarbons or halogenated hydrocarbons, either alone or in mixtures, such as pentane, hexane, heptane, cyclohexane, methylcyclohexane, benzene, toluene, ethylbenzene, xylene, mesitylene, limonene, chloro-substituted benzene, chloro-substituted toluene, methylene chloride, chloroform, etc. Preferably, mixed alkane solvents, cyclohexane, toluene, ethylbenzene, etc. can be used as the solvent.

[0086] Although the copolymer can be produced without using a chain transfer agent, a chain transfer agent may be used to reduce the molecular weight. Examples of such a chain transfer agent include known chain transfer agents used with so-called single-site coordination polymerization catalysts, such as hydrogen, alkyl aluminums such as triisobutylaluminum, and 9-BBN, as described in Chung TC: Macromolecules, 26, 3467 (1993).

[0087] The equipment capable of producing the present composition may be, for example, a single tank polymerization vessel or a plurality of connected tanks, or a linear or loop pipe polymerization vessel or a plurality of connected tanks. The pipe polymerization vessel may be equipped with various known mixers such as a dynamic or static mixer or a static mixer that also serves as a heat remover, or various known coolers such as a cooler equipped with a thin tube for heat removal. It may also be equipped with a batch-type prepolymerization vessel. Furthermore, a gas-phase polymerization process may be employed.

[0088] The polymerization temperature is preferably 0 to 200°C. A temperature of 0°C or higher is industrially advantageous because the polymerization rate is fast, while a temperature of 200°C or lower has the effect of making the transition metal compound less susceptible to decomposition. Industrially, a temperature of 30 to 160°C is more preferable, and 50 to 160°C is particularly preferable. The pressure during polymerization is generally preferably 1 to 100 atmospheres, more preferably 1 to 30 atmospheres, and industrially, most preferably 1 to 10 atmospheres.

[0089] Any process can be used to recover the copolymer from the reaction system after the polymerization is complete, and preferably, the steam stripping method or crumb foaming method, which are known as methods for recovering raw rubber, can be used. In laboratories, a method in which the copolymer is precipitated in a large amount of methanol, known as the methanol precipitation method, is generally convenient. Alternatively, without recovering the copolymer, the solvent and residual monomers can be removed in whole or in part from the polymerization solution by evaporation using a rotary evaporator, film evaporator, or the like, and the resulting solution can be diluted with a solvent and used as a varnish. [Example]

[0090] [Table 1]

[0091] [Table 2]

[0092] [Table 3]

[0093] [Table 4]

[0094] To verify the occurrence of gelation, an LDM polymerization solution was prepared according to the following procedure. Based on the manufacturing methods described in JP-A-9-40709, WO-00 / 37517, JP-A-2009-161743, and JP-A-2010-280771, dimethylmethylenebiscyclopentadienylzirconium dichloride was used as the catalyst, methylaluminoxane (Tosoh Finechem Corporation, MMAO-3A toluene solution) as the cocatalyst, cyclohexane as the solvent, and styrene, divinylbenzene (a mixture of meta- and para-divinylbenzene), and ethylene as the raw materials. A 10 L autoclave equipped with a stirrer and a heating / cooling jacket was used. The monomer amounts, ratios, polymerization pressure, and polymerization temperature were adjusted as needed to obtain copolymers with the compositions shown in Table 1. 1-Isopropanol was added to the resulting polymerization solution to obtain an LDM polymerization solution. Furthermore, the chelating agents shown in Tables 2 and 3 were added to the LDM polymerization solution, which was then stirred and subjected to the evaluation described below.

[0095] In Tables 2 and 3, the LDM polymerization solution is taken as 100 parts by mass, and the catalyst, co-catalyst, and chelating agent are shown as externally divided amounts. In addition, in Tables 2 and 3, when calculating the number of moles of MMAO, the molecular weight (58.02) is used as the average. m (100.10) n The calculation was made with m=n=1 and the value was 158.12.

[0096] The chelating agents used were as follows: Chelating agent 1: TBC (4-tert-butylcatechol, molecular weight 165.2) Chelating agent 2: Acac (acetylacetone, molecular weight 100.12) Chelating agent 3: AcacOEt (ethyl acetoacetate, molecular weight 130.14) Chelating agent 4: TMEDA (tetramethylethylenediamine, molecular weight 116.24) Chelating agent 5: EDTA·4Na (tetrasodium ethylenediaminetetraacetic acid, molecular weight 380.17)

[0097] The obtained polymer (composition) was exposed to the atmosphere, and after 5 hours, it was visually confirmed whether or not a gel had formed.

[0098] The viscosity of the resin solution containing the polymer obtained in each Example and Comparative Example was measured as follows. The resin solution was concentrated using a rotary evaporator and diluted with toluene to a concentration of 50% by mass to prepare a solution for measurement. The viscosity was measured using a rotational rheometer ("MCR302" manufactured by Anton Paar) at 25°C and a shear rate of 1 sec. -1 Furthermore, water was added to the polymer in an amount of 5000 ppm relative to the resin, and the viscosity was measured again in the same manner after 1 hour to confirm whether the viscosity had increased by 50% or more, and this was evaluated as "thickening upon addition of water" in the table.

[0099] Furthermore, for some of the compositions of the Examples and Comparative Examples, the components in the LDM polymerization solution were adjusted to 100 parts by mass according to the formulations shown in Table 4, and a toluene solvent and a curing agent (NOF Corporation's "Perhexyne 25B", 2,5-dimethyl-2,5-bis(tert-butylperoxy)hexyne-3) were further added, and coordination polymerization was carried out in the same manner as above to obtain polymers. The obtained polymers were evaluated as follows. The results are shown in Table 4.

[0100] <Measurement of storage modulus> Measurements were taken using a dynamic viscoelasticity measuring device (TA Instruments, formerly Rheometrics RSA-G2) at a frequency of 1 Hz and in the temperature range of -60°C to +300°C. Measurement samples (3mm x 40mm) were cut out from films approximately 0.1 to 0.3mm thick and measured to determine the storage modulus at 25°C. The main measurement parameters involved in the measurement are as follows: Measurement frequency 1Hz Heating rate: 3°C / min Sample measurement length: 10 mm Distortion 0.1%

[0101] <Measurement of dielectric constant and dielectric loss (dielectric loss tangent)> The dielectric constant and dielectric loss tangent were evaluated in the same manner using a balanced circular disk resonator (Keysight Technologies). To evaluate the dielectric properties of the balanced circular disk resonator, two samples (3 cm diameter, 0.2–0.6 mm thick) were cut from a sheet and placed inside the resonator with copper foil between them. The resonant frequency (f0) and unloaded Q value (Qu) of the peaks appearing between 27 and 42 GHz were measured. The dielectric constant was calculated from f0, and the dielectric loss tangent (tanδc) was calculated from Qu using the analysis software provided with the resonator (Balanced Type Circular Disk Resonator (Method) Calculator). The measurement temperature was 23°C and humidity was 50% RH.

[0102] As shown in Tables 2 and 3, neither Example 1, which used chelating agent 1 having two oxygen atoms in the molecule, nor Examples 2 to 6, which used chelating agent 2, showed any gel formation or increase in viscosity when water was added.

[0103] On the other hand, in Comparative Examples 1 and 7 to 8, in which no chelating agent was added, gel was generated and the viscosity increased when water was added.

[0104] In Comparative Example 2, the same chelating agent 1 as in Example 1 was used, but the amount was too small, resulting in the formation of a gel and an increase in viscosity when water was added, which was unsuitable.

[0105] In Comparative Example 3, which used chelating agent 3 having an ester structure with many oxygen atoms in the molecule, the dielectric loss tangent was higher than in the Examples, and was therefore unsuitable. Even a slight difference in the dielectric loss tangent (a difference on the order of 0.0001) can have a large effect, so even a slight decrease can have a significant effect.

[0106] In Comparative Example 4, which used chelating agent 4 having a nitrogen atom but no oxygen atom in the molecule, gelation occurred and the viscosity increased when water was added, which was unsuitable.

[0107] In Comparative Example 5, which used chelating agent 5 having many oxygen atoms and also nitrogen atoms in the molecule, the solubility of the chelating agent was poor, resulting in the formation of a gel and the viscosity increasing when water was added, which was unsuitable.

[0108] In Comparative Example 6, the same chelating agent 2 as in Examples 2 to 4 was used, but the amount was too small, resulting in the formation of a gel and an increase in viscosity when water was added, which was unsuitable.

Claims

1. (A) a curable hydrocarbon-based resin; (C) a co-catalyst containing at least one of an aluminum compound and a boron compound; (D) a chelating agent having one or two oxygen atoms in one molecule; (E) a catalyst that is a metal compound or a semimetal compound and does not contain the co-catalyst; A composition comprising: The amount of component (D) per 1 mol of component (C) contained in the composition is 2 mol or more. A composition characterized by:

2. 2. The composition according to claim 1, wherein component (A) comprises an olefin-aromatic vinyl compound-aromatic polyene copolymer.

3. 3. The composition according to claim 2, wherein component (A) satisfies the following conditions (1) to (4): (1) The number average molecular weight of the copolymer is 500 or more and 100,000 or less. (2) The aromatic vinyl compound monomer unit is an aromatic vinyl compound having 8 to 20 carbon atoms, and the content of the aromatic vinyl compound monomer unit is 0 to 70% by mass. (3) The aromatic polyene monomer unit is one or more polyenes selected from polyenes having 5 to 20 carbon atoms and having a plurality of vinyl groups and / or vinylene groups in the molecule, and the content of vinyl groups and / or vinylene groups derived from the aromatic polyene monomer unit is 1.5 or more and less than 20 per number average molecular weight. (4) The olefin monomer unit is one or more olefins selected from olefins having 2 to 20 carbon atoms, and the total of the olefin monomer units, aromatic vinyl compound monomer units, and aromatic polyene monomer units is 100% by mass.

4. (B) a resin component containing at least one selected from the group consisting of a thermoplastic hydrocarbon elastomer and a thermoplastic conjugated diene polymer; 3. The composition of claim 1 or 2, further comprising:

5. 3. The composition according to claim 1, wherein the amount of component (D) is 0.5 parts by mass or more and 10 parts by mass or less when component (A) is 100 parts by mass.

6. 3. The composition according to claim 1, wherein component (E) comprises at least one of a zirconium compound and a hafnium compound.

7. 7. The composition according to claim 6, wherein the amount of component (D) contained in the composition per 1 mole of component (E) is 100 mol or more.

8. 3. The composition according to claim 1, wherein component (D) does not contain a nitrogen atom in the molecule.

9. 3. The composition according to claim 1, wherein component (D) comprises one or more selected from the group consisting of 4-tert-butylcatechol and acetylacetone.

10. A cured product of the composition according to claim 1 or 2.

11. A laminate comprising a layer containing the composition according to claim 1 or 2 and a metal foil.

12. A single-layer CCL, multi-layer CCL, single-layer FCCL, or multi-layer FCCL substrate comprising the cured product according to claim 10.

13. A solution comprising the composition according to claim 1 or 2 and a solvent for dissolving the composition.

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