Compounds and moldings

Abstract

A compound comprising a metallic-element-containing powder and a resin composition, wherein the resin composition comprises an epoxy resin and one or more compounds each having a siloxane bond, the compounds having a siloxane bond being contained in an amount of 20 parts by mass or less per 100 parts by mass of the epoxy resin and including a siloxane compound having a structure represented by chemical formula (1).

Description

[Technical field]

[0001] The present invention relates to a compound and a molded article. [Background technology]

[0002] Compounds containing metal powder and a resin composition are used as raw materials for various industrial products such as inductors, electromagnetic shields, and bonded magnets, depending on the physical properties of the metal powder (see Patent Document 1 below). [Prior art documents] [Patent documents]

[0003] [Patent Document 1] JP 2014-13803 A Summary of the Invention [Problem to be solved by the invention]

[0004] Industrial products such as inductors may require resistance to heat and voltage. An object of the present invention is to provide a compound capable of obtaining a molded article having both heat resistance and voltage resistance, and a molded article including the compound. [Means for solving the problem]

[0005] A compound according to one aspect of the present invention comprises a metal element-containing powder and a resin composition, the resin composition containing an epoxy resin and a chemical compound having a siloxane bond, the content of the compound having a siloxane bond being 20 parts by mass or less per 100 parts by mass of the epoxy resin, and the compound having a siloxane bond including a siloxane compound having a structure represented by the following chemical formula (1): [ka] [In the above chemical formula (1), n ​​is an integer of 2 to 200, and R 1 and R2 Each of them is independently an alkyl group having 1 to 10 carbon atoms, an aryl group having 6 to 10 carbon atoms, an alkoxy group having 1 to 10 carbon atoms, a monovalent organic group having an epoxy group, a monovalent organic group having a carboxy group, or a polyalkylene ether group having 3 to 500 carbon atoms.]

[0006] In the compound according to one aspect of the present invention, the siloxane compound may further have a structural unit represented by the following chemical formula (2).

[0007] [ka] [In the above chemical formula (2), R 3 is an alkylene group having 1 to 10 carbon atoms.]

[0008] The compound according to one aspect of the present invention may contain a compound represented by the following chemical formula (3) as a siloxane compound.

[0009] [ka] [In the above chemical formula (3), n is an integer of 2 to 200, and m 1 and m 2 each independently represents an integer from 1 to 200; R 4 , R 5 , R 6 and R 7 each independently represents an alkyl group having 1 to 10 carbon atoms, an aryl group having 6 to 10 carbon atoms, an alkoxy group having 1 to 10 carbon atoms, a monovalent organic group having an epoxy group, a monovalent organic group having a carboxy group, or a polyalkylene ether group having 3 to 500 carbon atoms; R 8 and R 9 each independently represents an alkylene group having 1 to 10 carbon atoms; R 10 and R 11 Each of them is independently a divalent hydrocarbon group having 1 to 10 carbon atoms which may contain an ether structure.]

[0010] The compound according to one aspect of the present invention may contain, as an epoxy resin, at least one of a biphenylene aralkyl type epoxy resin and an isocyanate-modified epoxy resin.

[0011] In the compound according to one aspect of the present invention, the content of the metal element-containing powder may be equal to or greater than 90% by mass and less than 100% by mass.

[0012] A molded article according to one aspect of the present invention includes the above-mentioned compound. Effect of the Invention

[0013] According to the present invention, there is provided a compound capable of obtaining a molded article having both heat resistance and voltage resistance, and a molded article including the compound. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0014] Preferred embodiments of the present invention will be described below, however, the present invention is not limited to the following embodiments.

[0015] <Compound Overview> The compound according to the present embodiment includes a metal element-containing powder and a resin composition. The metal element-containing powder is composed of a plurality (a large number) of metal element-containing particles. The metal element-containing powder (metal element-containing particles) may contain at least one selected from the group consisting of a simple metal, an alloy, and a metal compound. The resin composition contains at least an epoxy resin and a compound having a siloxane bond. The compound having a siloxane bond may be written as a "siloxane compound". The resin composition may contain other components in addition to the epoxy resin and the siloxane compound. For example, the resin composition may contain a curing agent. The resin composition may contain a curing accelerator. The resin composition may contain an additive. The resin composition may be a component that may include an epoxy resin, a siloxane compound, a curing agent, a curing accelerator, and an additive, and may be the remaining components (non-volatile components) excluding the organic solvent and the metal element-containing powder. The additive is the remaining component of the resin composition excluding the resin, the siloxane compound, the curing agent, and the curing accelerator. The additive is, for example, a coupling agent or a flame retardant. The resin composition may contain a wax as an additive. The compound may be a powder (compound powder).

[0016] The compound according to the present embodiment contains a predetermined amount of a siloxane compound, which is a type of elastomer. The reason why the heat resistance and voltage resistance of the molded body obtained from the compound are improved by the addition of a predetermined amount of the siloxane compound is not clear, but the inventors speculate that the following possibilities are the cause. First, it is believed that the addition of the siloxane compound improves the fluidity of the contained components, thereby suppressing the generation of internal voids during molding. Second, it is believed that the compatibility between the metal element-containing powder and the epoxy resin is low, and the interface between the two is thought to cause a decrease in characteristics, but the addition of the siloxane compound improves the compatibility between the two. However, the effects of the present invention are not limited to the above.

[0017] The compound may comprise a metal element-containing powder and a resin composition attached to the surface of each metal element-containing particle constituting the metal element-containing powder. The resin composition may cover the entire surface of the particle, or may cover only a part of the surface of the particle. The compound may comprise an uncured resin composition and a metal element-containing powder. The compound may comprise a semi-cured product of the resin composition (e.g., a B-stage resin composition) and a metal element-containing powder. The compound may comprise both an uncured resin composition and a semi-cured product of the resin composition. The compound may be composed of a metal element-containing powder and a resin composition.

[0018] The content of the metal element-containing powder in the compound may be 90% by mass or more and less than 100% by mass, 90% by mass or more and 99.8% by mass or less, 92% by mass or more and 99.5% by mass or less, 94% by mass or more and 98.5% by mass or less, or 94% by mass or more and 97.5% by mass or less, based on the mass of the entire compound. In addition to the metal element-containing powder, the compound may contain other fillers (e.g., silica filler).

[0019] The content of the resin composition in the compound may be 0.2 mass% or more and 10 mass% or less, or 4 mass% or more and 6 mass% or less, based on the total mass of the compound (for example, the total mass of the metal element-containing powder and the resin composition).

[0020] The content of the siloxane compound in the compound is 20 parts by mass or less, but may be 17.5 parts by mass or less, or 15 parts by mass or less, relative to 100 parts by mass of the epoxy resin. When the content of the siloxane compound is within the above range, the heat resistance and voltage resistance of the molded body are compatible. On the other hand, the lower limit of the content of the siloxane compound in the compound is not particularly limited, but from the viewpoint of moldability, etc., it may be 0.1 parts by mass or more, 5 parts by mass or more, 7.5 parts by mass or more, or 10 parts by mass or more, relative to 100 parts by mass of the epoxy resin.

[0021] The average particle size of the metal element-containing powder is not particularly limited, but may be, for example, 1 μm or more and 300 μm or less. The average particle size may be measured, for example, by a particle size distribution meter. The shape of each metal element-containing particle constituting the metal element-containing powder is not limited, but may be, for example, spherical, flat, prismatic, or acicular. The compound may include a plurality of types of metal element-containing powders having different average particle sizes.

[0022] Depending on the composition or combination of the metal element-containing powder contained in the compound, the various properties such as the electromagnetic properties of the molded body formed from the compound can be freely controlled, and the molded body can be used as various industrial products or their raw materials. The industrial products manufactured using the compound may be, for example, automobiles, medical devices, electronic devices, electric devices, information and communication devices, home appliances, audio devices, and general industrial devices. For example, when the compound contains a permanent magnet such as an Sm-Fe-N alloy or an Nd-Fe-B alloy as the metal element-containing powder, the compound may be used as a raw material for a bonded magnet. When the compound contains a soft magnetic powder such as an Fe-Si-Cr alloy or ferrite as the metal element-containing powder, the compound may be used as a raw material for an inductor (e.g., an EMI filter) or a transformer (e.g., a magnetic core). When the compound contains iron and copper as the metal element-containing powder, the molded body (e.g., a sheet) formed from the compound may be used as an electromagnetic wave shield.

[0023] <Compound composition> (Resin composition) The resin composition functions as a binder for the metal element-containing particles that constitute the metal element-containing powder, and imparts mechanical strength to a molded body formed from the compound. For example, when the compound is molded under high pressure using a mold, the resin composition fills between the metal element-containing particles and binds the metal element-containing particles to each other. By curing the resin composition in the molded body, the cured resin composition binds the metal element-containing particles to each other more firmly, improving the mechanical strength of the molded body.

[0024] The resin composition contains at least an epoxy resin as a thermosetting resin. The compound contains an epoxy resin, which has relatively excellent fluidity among thermosetting resins, and thus the fluidity, storage stability, and moldability of the compound are improved. However, the compound may contain other resins in addition to the epoxy resin, as long as the effects of the present invention are not impaired. For example, the resin composition may contain at least one of a phenolic resin and a polyamide-imide resin as a thermosetting resin. When the resin composition contains both an epoxy resin and a phenolic resin, the phenolic resin may function as a curing agent for the epoxy resin. The resin composition may contain a thermoplastic resin. The thermoplastic resin may be, for example, at least one selected from the group consisting of an acrylic resin, polyethylene, polypropylene, polystyrene, polyvinyl chloride, and polyethylene terephthalate. The resin composition may contain both a thermosetting resin and a thermoplastic resin. The resin composition may contain a silicone resin.

[0025] The epoxy resin may be, for example, a resin having two or more epoxy groups in one molecule. The epoxy resin may be, for example, a resin having three or more epoxy groups in one molecule. The epoxy resin may be a polyfunctional epoxy resin. The epoxy resin may be, for example, a biphenyl type epoxy resin, a stilbene type epoxy resin, a diphenylmethane type epoxy resin, a sulfur atom-containing epoxy resin, a novolac type epoxy resin, a dicyclopentadiene type epoxy resin, a salicylaldehyde type epoxy resin, a copolymer type epoxy resin of naphthols and phenols, an epoxidized product of an aralkyl type phenolic resin, a bisphenol type epoxy resin, an epoxy resin containing a bisphenol skeleton, a glycidyl ether type epoxy resin of alcohols, a glycidyl ether type epoxy resin of a paraxylylene and / or a metaxylylene modified phenolic resin, a glycidyl ether type epoxy resin of a terpene modified phenolic resin, or a glycidyl ether type epoxy resin of a terpene modified phenolic resin. and the like. The epoxy resin may be at least one selected from the group consisting of glycidyl ether type epoxy resins, cyclopentadiene type epoxy resins, glycidyl ether type epoxy resins of polycyclic aromatic ring-modified phenolic resins, glycidyl ether type epoxy resins of naphthalene ring-containing phenolic resins, glycidyl ester type epoxy resins, glycidyl or methylglycidyl type epoxy resins, alicyclic type epoxy resins, halogenated phenol novolac type epoxy resins, ortho-cresol novolac type epoxy resins, hydroquinone type epoxy resins, trimethylolpropane type epoxy resins, and linear aliphatic epoxy resins obtained by oxidizing an olefin bond with a peracid such as peracetic acid.

[0026] From the viewpoint of excellent fluidity, the epoxy resin may be at least one selected from the group consisting of biphenyl type epoxy resins, orthocresol novolac type epoxy resins, phenol novolac type epoxy resins, bisphenol type epoxy resins, epoxy resins having a bisphenol skeleton, salicylaldehyde novolac type epoxy resins, and naphthol novolac type epoxy resins.

[0027] The epoxy resin may be a crystalline epoxy resin. Although the molecular weight of the crystalline epoxy resin is relatively low, the crystalline epoxy resin has a relatively high melting point and excellent fluidity. The crystalline epoxy resin (highly crystalline epoxy resin) may be, for example, at least one selected from the group consisting of hydroquinone type epoxy resin, bisphenol type epoxy resin, thioether type epoxy resin, and biphenyl type epoxy resin. Commercially available crystalline epoxy resins include, for example, Epicron 860, Epicron 1050, Epicron 1055, Epicron 2050, Epicron 3050, Epicron 4050, Epicron 7050, Epicron HM-091, Epicron HM-101, Epicron N-730A, Epicron N-740, Epicron N-770, Epicron N-775, Epicron N-776, Epicron N-777, Epicron N-778, Epicron N-779, Epicron N-780, Epicron N-781, Epicron N-782, Epicron N-783, Epicron N-784, Epicron N-785, Epicron N-786, Epicron N-787, Epicron N-788, Epicron N-789 ...9, Epicron N-789, Epicron N-789, Epicron N-789, Epicron N-789, Epicron N-789, Epicron N-789, Epicron N-789, Clon N-865, Epiclon HP-4032D, Epiclon HP-7200L, Epiclon HP-7200, Epiclon HP-7200H, Epiclon HP-7200HH, Epiclon HP-7200HHH, Epiclon HP-4700, Epiclon HP-4710, Epiclon HP-4770, Epiclon HP-5000, Epiclon HP-6000, N 500P-2, and N500P-10 (all product names manufactured by DIC Corporation), NC-3000, NC-3000-L, NC-3000-H, NC-3100, CER-3000- L, NC-2000-L, XD-1000, NC-7000-L, NC-7300-L, EPPN-501H, EPPN-501HY, EPPN-502H, EOCN-1020, It may be at least one selected from the group consisting of EOCN-102S, EOCN-103S, EOCN-104S, CER-1020, EPPN-201, BREN-S, BREN-10S (all of which are trade names manufactured by Nippon Kayaku Co., Ltd.), YX-4000, YX-4000H, YL4121H, and YX-8800 (all of which are trade names manufactured by Mitsubishi Chemical Corporation).

[0028] From the viewpoint of easily reducing the molding shrinkage rate of the compound and easily improving the heat resistance and voltage resistance of the molded body, the resin composition may contain at least one of biphenylene aralkyl type epoxy resin and isocyanate modified epoxy resin as the epoxy resin. The resin composition may contain both biphenylene aralkyl type epoxy resin and isocyanate modified epoxy resin as the epoxy resin. A commercially available product of biphenylene aralkyl type epoxy resin may be, for example, NC-3000 manufactured by Nippon Kayaku Co., Ltd. A commercially available product of isocyanate modified epoxy resin may be, for example, AER-4001 manufactured by Asahi Kasei Corporation (formerly Asahi Kasei E-Materials Co., Ltd.). From the viewpoint of easily improving the heat resistance and voltage resistance of the molded body, the resin composition may contain a multifunctional epoxy resin. A commercially available product of multifunctional epoxy resin may be, for example, VG-3101L manufactured by Printec Co., Ltd.

[0029] The resin composition may contain one type of epoxy resin among the above-mentioned epoxy resins. The resin composition may contain two or more types of epoxy resins among the above-mentioned epoxy resins.

[0030] Curing agents are classified into those that cure epoxy resins at temperatures ranging from low to room temperature, and heat-curing curing agents that cure epoxy resins by heating. Examples of curing agents that cure epoxy resins at temperatures ranging from low to room temperature include aliphatic polyamines, polyaminoamides, and polymercaptans. Examples of heat-curing curing agents include aromatic polyamines, acid anhydrides, phenol novolac resins, and dicyandiamide (DICY).

[0031] When a curing agent that cures an epoxy resin in the range of low temperature to room temperature is used, the glass transition point of the cured product of the epoxy resin is low, and the cured product of the epoxy resin tends to be soft. As a result, the molded product formed from the compound also tends to be soft. On the other hand, from the viewpoint of improving the heat resistance of the molded product, the curing agent may be preferably a heat-curing type curing agent, more preferably a phenolic resin, and even more preferably a phenolic novolac resin. In particular, by using a phenolic novolac resin as a curing agent, it is easy to obtain a cured product of an epoxy resin with a high glass transition point. As a result, the heat resistance and mechanical strength of the molded product are easily improved.

[0032] The phenolic resin may be at least one selected from the group consisting of, for example, aralkyl type phenolic resin, dicyclopentadiene type phenolic resin, salicylaldehyde type phenolic resin, novolac type phenolic resin, copolymer type phenolic resin of benzaldehyde type phenol and aralkyl type phenol, paraxylylene and / or metaxylylene modified phenolic resin, melamine modified phenolic resin, terpene modified phenolic resin, dicyclopentadiene type naphthol resin, cyclopentadiene modified phenolic resin, polycyclic aromatic ring modified phenolic resin, biphenyl type phenolic resin, and triphenylmethane type phenolic resin. The phenolic resin may be a copolymer composed of two or more of the above. As a commercially available product of the phenolic resin, for example, Tamanoru 758 manufactured by Arakawa Chemical Industries Co., Ltd., or HP-850N manufactured by Hitachi Chemical Co., Ltd. may be used.

[0033] The phenol novolac resin may be, for example, a resin obtained by condensing or co-condensing phenols and / or naphthols with aldehydes under an acid catalyst. The phenols constituting the phenol novolac resin may be, for example, at least one selected from the group consisting of phenol, cresol, xylenol, resorcin, catechol, bisphenol A, bisphenol F, phenylphenol, and aminophenol. The naphthols constituting the phenol novolac resin may be, for example, at least one selected from the group consisting of α-naphthol, β-naphthol, and dihydroxynaphthalene. The aldehydes constituting the phenol novolac resin may be, for example, at least one selected from the group consisting of formaldehyde, acetaldehyde, propionaldehyde, benzaldehyde, and salicylaldehyde. Commercially available phenol novolac resins include, for example, HF-3M and MEW-1800 manufactured by Meiwa Kasei Co., Ltd.

[0034] The curing agent may be, for example, a compound having two phenolic hydroxyl groups in one molecule. The compound having two phenolic hydroxyl groups in one molecule may be, for example, at least one selected from the group consisting of resorcin, catechol, bisphenol A, bisphenol F, and substituted or unsubstituted biphenol.

[0035] The resin composition may contain one type of phenolic resin from among the above. The resin composition may comprise a plurality of types of phenolic resins from among the above. The resin composition may contain one type of curing agent from among the above. The resin composition may contain a plurality of types of curing agents from among the above.

[0036] The ratio of the active group (phenolic OH group) in the curing agent that reacts with the epoxy group in the epoxy resin may be preferably 0.5 to 1.5 equivalents, more preferably 0.6 to 1.4 equivalents, and even more preferably 0.8 to 1.2 equivalents relative to 1 equivalent of the epoxy group in the epoxy resin. If the ratio of the active group in the curing agent is less than 0.5 equivalents, it is difficult to obtain a sufficient elastic modulus of the obtained cured product. On the other hand, if the ratio of the active group in the curing agent exceeds 1.5 equivalents, the mechanical strength of the molded product formed from the compound after curing tends to decrease. However, even if the ratio of the active group in the curing agent is outside the above range, the effect of the present invention can be obtained.

[0037] The curing accelerator (catalyst) is not limited as long as it is a composition that reacts with an epoxy resin to accelerate the curing of the epoxy resin. The curing accelerator may be, for example, an imidazole such as an alkyl group-substituted imidazole or benzimidazole. The resin composition may include one type of curing accelerator. The resin composition may include multiple types of curing accelerators. When the resin composition contains a curing accelerator, the moldability and releasability of the compound are easily improved. In addition, when the resin composition contains a curing accelerator, the mechanical strength of a molded body (e.g., electronic parts) manufactured using the compound is improved, and the storage stability of the compound under high temperature and high humidity environments is improved. As a commercially available product of the imidazole-based curing accelerator, for example, at least one selected from the group consisting of 2MZ-H, C11Z, C17Z, 1,2DMZ, 2E4MZ, 2PZ-PW, 2P4MZ, 1B2MZ, 1B2PZ, 2MZ-CN, C11Z-CN, 2E4MZ-CN, 2PZ-CN, C11Z-CNS, 2P4MHZ, TPZ, and SFZ (all trade names of Shikoku Chemical Industry Co., Ltd.) may be used. As a curing accelerator (catalyst), for example, a urea-based catalyst may be used. As a commercially available product of the urea-based catalyst, for example, U-CAT3512T manufactured by San-Apro Co., Ltd. may be used.

[0038] The amount of the curing accelerator is not particularly limited as long as it is an amount that can obtain a curing acceleration effect. However, from the viewpoint of improving the curability and fluidity of the resin composition when absorbing moisture, the amount of the curing accelerator may be preferably 0.1 parts by mass or more and 30 parts by mass or less, more preferably 1 part by mass or more and 15 parts by mass or less, relative to 100 parts by mass of the epoxy resin. The content of the curing accelerator is preferably 0.001 parts by mass or more and 5 parts by mass or less, relative to 100 parts by mass of the total mass of the epoxy resin and the curing agent (e.g., phenolic resin). When the amount of the curing accelerator is less than 0.1 parts by mass, it is difficult to obtain a sufficient curing acceleration effect. When the amount of the curing accelerator is more than 30 parts by mass, the storage stability of the compound is easily reduced. However, even if the amount and content of the curing accelerator are outside the above range, the effect of the present invention can be obtained.

[0039] The resin composition contains a compound having a siloxane bond (siloxane compound). The siloxane bond is a bond containing two silicon atoms (Si) and one oxygen atom (O), and may be represented by -Si-O-Si-. The compound having a siloxane bond may be a polysiloxane compound. The resin composition may contain one type of siloxane compound, or may contain multiple types of siloxane compounds. From the viewpoint of easily reducing the molding shrinkage rate of the compound and easily improving the heat resistance and voltage resistance of the molded body, it is preferable that the resin composition contains a first siloxane compound described later as the siloxane compound. The resin composition may contain only the first siloxane compound as the siloxane compound, or may further contain a second siloxane compound. The resin composition may contain both the first siloxane compound and the second siloxane compound. The resin composition may contain a siloxane compound other than the first siloxane compound and the second siloxane compound. The first siloxane compound and the second siloxane compound will be described in detail below.

[0040] The first siloxane compound may have a structural unit represented by the following chemical formula (1). The structural unit may simply be referred to as a "structure." The structural unit represented by the following chemical formula (1) may be referred to as "structural unit 1."

[0041] [ka]

[0042] In the above chemical formula (1), n ​​is an integer of 2 to 200, and R 1 and R 2 Each of them is independently an alkyl group having 1 to 10 carbon atoms, an aryl group having 6 to 10 carbon atoms, an alkoxy group having 1 to 10 carbon atoms, a monovalent organic group having an epoxy group, a monovalent organic group having a carboxy group, or a polyalkylene ether group having 3 to 500 carbon atoms.

[0043] The plurality of R present in the first siloxane compound 1 may be the same or different. 2 may be the same or different. 1 and R 2 may be the same or different. The first siloxane compound may have a repeating unit represented by the above chemical formula (1).

[0044] From the viewpoint of easily reducing the molding shrinkage rate of the compound and easily improving the heat resistance and voltage resistance of the molded article, it is preferable that the first siloxane compound further has a structural unit represented by the following chemical formula (2). The structural unit represented by the following chemical formula (2) may be referred to as "structural unit 2".

[0045] [ka]

[0046] In the above chemical formula (2), R 3 is an alkylene group having 1 to 10 carbon atoms.

[0047] The first siloxane compound may have a plurality of structural units 2. 3may be the same or different. The first siloxane compound may have a repeating unit represented by the above chemical formula (2).

[0048] From the viewpoint of easily reducing the molding shrinkage rate of the compound and easily improving the heat resistance and voltage resistance of the molded body, the first siloxane compound is preferably a compound represented by the following chemical formula (3). The compound represented by the following chemical formula (3) may be referred to as "compound 3".

[0049] [ka]

[0050] In the above chemical formula (3), n is an integer of 2 to 200. 1 and m 2 Each is independently an integer from 1 to 200. 4 , R 5 , R 6 and R 7 Each of them is independently an alkyl group having 1 to 10 carbon atoms, an aryl group having 6 to 10 carbon atoms, an alkoxy group having 1 to 10 carbon atoms, a monovalent organic group having an epoxy group, a monovalent organic group having a carboxy group, or a polyalkylene ether group having 3 to 500 carbon atoms. 8 and R 9 Each of them is independently an alkylene group having 1 to 10 carbon atoms. 10 and R 11 Each of R is independently a divalent hydrocarbon group having 1 to 10 carbon atoms which may contain an ether structure. 10 and R 11 It can also be said that each of them is independently a divalent hydrocarbon group having 1 to 10 carbon atoms which may contain an oxygen atom or which may be bonded via an oxygen atom.

[0051] Multiple R present in compound 3 4 may be the same or different. 5 may be the same or different. 4 , R 5 , R 6and R 7 may be the same or different. 8 may be the same or different. 9 may be the same or different. 8 and R 9 may be the same or different. The weight average molecular weight (Mw) of compound 3 may be, for example, 4,000 or more and 20,000 or less.

[0052] Commercially available products of compound 3 include, for example, DBL-C31 and DBL-C32 manufactured by Gelest Corporation.

[0053] From the viewpoint of easily reducing the molding shrinkage rate of the compound and easily improving the heat resistance and voltage resistance of the molded body, the second siloxane compound preferably has a structural unit represented by the following chemical formula (4) and a structural unit represented by the following chemical formula (5). The structural unit represented by the following chemical formula (4) may be expressed as "structural unit 4". The structural unit represented by the following chemical formula (5) may be expressed as "structural unit 5".

[0054] [ka]

[0055] In the above chemical formula (4), R 12 R is a monovalent hydrocarbon group having 1 to 12 carbon atoms. 17 is an organic group having one or more carbon atoms.

[0056] R 12 R may be, for example, an alkyl group such as a methyl group, an ethyl group, a propyl group, a butyl group, an isopropyl group, an isobutyl group, a t-butyl group, a pentyl group, a hexyl group, a heptyl group, an octyl group, or a 2-ethylhexyl group; an alkenyl group such as a vinyl group, an allyl group, a butenyl group, a pentenyl group, or a hexenyl group; an aryl group such as a phenyl group, a tolyl group, a xylyl group, a naphthyl group, or a biphenyl group; or an aralkyl group such as a benzyl group or a phenethyl group. 12is preferably a methyl group or a phenyl group.

[0057] The second siloxane compound may have a plurality of structural units 4. 12 may be the same or different. The second siloxane compound may have a repeating unit represented by the above chemical formula (4).

[0058] [ka]

[0059] In the above chemical formula (5), R 13 and R 14 Each is independently a monovalent hydrocarbon group having 1 to 12 carbon atoms.

[0060] R 13 R may be, for example, an alkyl group such as a methyl group, an ethyl group, a propyl group, a butyl group, an isopropyl group, an isobutyl group, a t-butyl group, a pentyl group, a hexyl group, a heptyl group, an octyl group, or a 2-ethylhexyl group; an alkenyl group such as a vinyl group, an allyl group, a butenyl group, a pentenyl group, or a hexenyl group; an aryl group such as a phenyl group, a tolyl group, a xylyl group, a naphthyl group, or a biphenyl group; or an aralkyl group such as a benzyl group or a phenethyl group. 13 is preferably a methyl group or a phenyl group.

[0061] R 14 R may be, for example, an alkyl group such as a methyl group, an ethyl group, a propyl group, a butyl group, an isopropyl group, an isobutyl group, a t-butyl group, a pentyl group, a hexyl group, a heptyl group, an octyl group, or a 2-ethylhexyl group; an alkenyl group such as a vinyl group, an allyl group, a butenyl group, a pentenyl group, or a hexenyl group; an aryl group such as a phenyl group, a tolyl group, a xylyl group, a naphthyl group, or a biphenyl group; or an aralkyl group such as a benzyl group or a phenethyl group. 14 is preferably a methyl group or a phenyl group.

[0062] The second siloxane compound may have a plurality of structural units 5. The plurality of R 13 may be the same or different. 14 may be the same or different. 13 and R 14 may be the same or different. The second siloxane compound may have a repeating unit represented by the above chemical formula (5).

[0063] From the viewpoint of storage stability of the second siloxane compound, the end of the molecule of the second siloxane compound is R 12 , R 13 , R 14 Preferably, the alkoxy group is any one of a hydroxyl group and an alkoxy group. The alkoxy group may be, for example, a methoxy group, an ethoxy group, a propoxy group, or a butoxy group.

[0064] From the viewpoint of easily reducing the molding shrinkage rate of the compound and easily improving the heat resistance and voltage resistance of the molded body, the second siloxane compound preferably has a structural unit represented by the following chemical formula (6): The structural unit represented by the following chemical formula (6) may be referred to as "structural unit 6".

[0065] [ka]

[0066] In the above chemical formula (6), R 15 R is a monovalent hydrocarbon group having 1 to 12 carbon atoms. 16 is a monovalent organic group having an epoxy group.

[0067] R 15R may be, for example, an alkyl group such as a methyl group, an ethyl group, a propyl group, a butyl group, an isopropyl group, an isobutyl group, a t-butyl group, a pentyl group, a hexyl group, a heptyl group, an octyl group, or a 2-ethylhexyl group; an alkenyl group such as a vinyl group, an allyl group, a butenyl group, a pentenyl group, or a hexenyl group; an aryl group such as a phenyl group, a tolyl group, a xylyl group, a naphthyl group, or a biphenyl group; or an aralkyl group such as a benzyl group or a phenethyl group. 13 is preferably a methyl group or a phenyl group.

[0068] R 16 R may be, for example, a 2,3-epoxypropyl group, a 3,4-epoxybutyl group, a 4,5-epoxypentyl group, a 2-glycidoxyethyl group, a 3-glycidoxypropyl group, a 4-glycidoxybutyl group, a 2-(3,4-epoxycyclohexyl)ethyl group, a 3-(3,4-epoxycyclohexyl)propyl group, and the like. 16 is preferably a 3-glycidoxypropyl group.

[0069] The second siloxane compound may have a plurality of structural units 6. 15 may be the same or different. 16 may be the same or different. The second siloxane compound may have a repeating unit represented by the above chemical formula (6).

[0070] From the viewpoint of easily reducing the molding shrinkage rate of the compound and easily improving the heat resistance and voltage resistance of the molded body, the second siloxane compound is preferably a compound having at least one structural unit selected from the group consisting of a structural unit represented by the following chemical formula (7), a structural unit represented by the following chemical formula (8), a structural unit represented by the following chemical formula (9), and a structural unit represented by the following chemical formula (10). The structural unit represented by the following chemical formula (7) may be expressed as "structural unit 7". The structural unit represented by the following chemical formula (8) may be expressed as "structural unit 8". The structural unit represented by the following chemical formula (9) may be expressed as "structural unit 9". The structural unit represented by the following chemical formula (10) may be expressed as "structural unit 10". A compound having at least one structural unit selected from the group consisting of the structural unit 7, the structural unit 8, the structural unit 9, and the structural unit 10 may be expressed as "compound 11". Compound 11 may have all of the structural units 7, 8, 9, and 10.

[0071] [ka]

[0072] [ka]

[0073] [ka] In the above chemical formula (9), R 18 is an organic group having one or more carbon atoms.

[0074] [ka] In the above chemical formula (10), R 19 is an organic group having one or more carbon atoms.

[0075] Compound 11 may have a plurality of structural units 7. Compound 11 may have a repeating unit represented by the above chemical formula (7). Compound 11 may have a plurality of structural units 8. Compound 11 may have a repeating unit represented by the above chemical formula (8). Compound 11 may have a plurality of structural units 9. Compound 11 may have a repeating unit represented by the above chemical formula (9). Compound 11 may have a plurality of structural units 10. Compound 11 may have a repeating unit represented by the above chemical formula (10).

[0076] A commercially available product of Compound 11 may be, for example, AY42-119 manufactured by Dow Corning Toray Co., Ltd.

[0077] The epoxy equivalent of the second siloxane compound may be from 500 to 4000, or from 1000 to 2500. When the epoxy equivalent is within the above range, the fluidity of the compound is likely to be improved, and the moldability is likely to be improved.

[0078] The softening point of the second siloxane compound is preferably 40°C or more and 120°C or less, more preferably 50°C or more and 100°C or less. When the softening point is within the above range, the mechanical strength of the molded body formed from the compound is easily improved. The softening point of the second siloxane compound may be adjusted by the molecular weight, structure (for example, the content ratio of each constituent unit), type of organic group bonded to silicon atom, etc. of the second siloxane compound. From the viewpoint of improving the fluidity of the compound, it is preferable to adjust the softening point by the content of aryl groups in the second siloxane compound. The aryl group may be, for example, a phenyl group, a tolyl group, a xylyl group, a naphthyl group, a biphenyl group, etc. The aryl group is preferably a phenyl group. It is more preferable to adjust the softening point by the content of phenyl groups in the monovalent organic group bonded to silicon atom in the second siloxane compound. The content of the phenyl group may be preferably adjusted to 60 mol% or more and 100 mol% or less, more preferably 70 mol% or more and 85 mol% or less.

[0079] The weight average molecular weight (Mw) of the second siloxane compound may be 1000 or more and 30000 or less, preferably 2000 or more and 20000 or less, more preferably 3000 or more and 10000 or less. The weight average molecular weight (Mw) may be measured by gel permeation chromatography (GPC) and may be a value converted using a standard polystyrene calibration curve. The second siloxane compound is preferably a random copolymer.

[0080] The resin composition may contain one type of siloxane compound among the above, or may contain a plurality of types of siloxane compounds among the above.

[0081] The coupling agent improves the adhesion between the resin composition and the metal element-containing particles constituting the metal element-containing powder, and improves the flexibility and mechanical strength of the molded body formed from the compound. The coupling agent may be, for example, at least one selected from the group consisting of silane-based compounds (silane coupling agents), titanium-based compounds, aluminum compounds (aluminum chelates), and aluminum / zirconium-based compounds. The silane coupling agent may be, for example, at least one selected from the group consisting of epoxy silane, mercapto silane, amino silane, alkyl silane, ureido silane, acid anhydride silane, and vinyl silane. In particular, aminophenyl-based silane coupling agents are preferred. The resin composition may contain one of the above coupling agents, or may contain multiple of the above coupling agents.

[0082] For the purpose of improving the environmental safety, recyclability, moldability and low cost of the compound, the compound may contain a flame retardant. The flame retardant may be, for example, at least one selected from the group consisting of bromine-based flame retardants, bulb flame retardants, hydrated metal compound-based flame retardants, silicone-based flame retardants, nitrogen-containing compounds, hindered amine compounds, organometallic compounds and aromatic engineering plastics. The resin composition may contain one of the above flame retardants or may contain multiple of the above flame retardants.

[0083] When a molded body is formed from the compound using a mold, the resin composition may contain a wax. The wax increases the fluidity of the compound during molding (e.g., transfer molding) of the compound and also functions as a mold release agent. The wax may be at least one of a fatty acid such as a higher fatty acid and a fatty acid ester.

[0084] Examples of the wax include fatty acids such as montanic acid, stearic acid, 12-hydroxystearic acid, and lauric acid, and esters thereof; fatty acid salts such as zinc stearate, calcium stearate, barium stearate, aluminum stearate, magnesium stearate, calcium laurate, zinc linoleate, calcium ricinoleate, and zinc 2-ethylhexanoate; and fatty acid salts such as stearic acid amide, oleic acid amide, erucic acid amide, behenic acid amide, palmitic acid amide, lauric acid amide, hydroxystearic acid amide, methylene bisstearic acid amide, ethylene bisstearic acid amide, ethylene bislauric acid amide, distearyl adipate amide, ethylene bisoleic acid amide, dioleyl adipate amide, N-stearyl stearic acid amide. The wax may be at least one selected from the group consisting of fatty acid amides such as butyl stearate, N-oleyl stearamide, N-stearyl erucamide, methylol stearamide, and methylol behenamide; fatty acid esters such as butyl stearate; alcohols such as ethylene glycol and stearyl alcohol; polyethers such as polyethylene glycol, polypropylene glycol, and polytetramethylene glycol and modified products thereof; silicone compounds such as silicone oil and silicone grease; fluorine compounds such as fluorine-based oil, fluorine-based grease, and fluorine-containing resin powder; and waxes such as paraffin wax, polyethylene wax, amide wax, polypropylene wax, ester wax, carnauba wax, and microwax. For example, a commercially available product of Montan acid ester is LICOWAX-OP manufactured by Clariant Chemicals Co., Ltd. For example, a commercially available product of natural wax is Carnauba Wax No. 1 manufactured by Cerarica NODA Co., Ltd.

[0085] Other examples of the release agent include metal soaps formed by bonding a metal with a long-chain fatty acid such as montanic acid, stearic acid, 12-oxystearic acid, or lauric acid. Commercially available metal soaps include Powder Base L manufactured by NOF Corporation.

[0086] (Powder containing metal elements) The metal element-containing powder (metal element-containing particle) may contain at least one selected from the group consisting of, for example, a metal element, an alloy, and a metal compound. The metal element-containing powder may be, for example, at least one selected from the group consisting of a metal element, an alloy, and a metal compound. The alloy may contain at least one selected from the group consisting of a solid solution, a eutectic, and an intermetallic compound. The alloy may be, for example, stainless steel (Fe-Cr alloy, Fe-Ni-Cr alloy, etc.). The metal compound may be, for example, an oxide such as ferrite. The metal element-containing powder may contain one type of metal element or multiple types of metal elements. The metal element contained in the metal element-containing powder may be, for example, a base metal element, a precious metal element, a transition metal element, or a rare earth element. The compound may contain one type of metal element-containing powder, or may contain multiple types of metal element-containing powders with different compositions.

[0087] The metal element-containing powder is not limited to the above composition. The metal element contained in the metal element-containing powder may be, for example, at least one selected from the group consisting of iron (Fe), copper (Cu), titanium (Ti), manganese (Mn), cobalt (Co), nickel (Ni), zinc (Zn), aluminum (Al), tin (Sn), chromium (Cr), barium (Ba), strontium (Sr), lead (Pb), silver (Ag), praseodymium (Pr), neodymium (Nd), samarium (Sm) and dysprosium (Dy). The metal element-containing powder may further contain elements other than the metal element. The metal element-containing powder may contain, for example, oxygen (O), beryllium (Be), phosphorus (P), boron (B), or silicon (Si). The metal element-containing powder may be a magnetic powder. The metal element-containing powder may be a soft magnetic alloy or a ferromagnetic alloy. The metal element-containing powder may be, for example, a magnetic powder consisting of at least one selected from the group consisting of Fe-Si alloy, Fe-Si-Al alloy (Sendust), Fe-Ni alloy (Permalloy), Fe-Cu-Ni alloy (Permalloy), Fe-Co alloy (Permendur), Fe-Cr-Si alloy (electromagnetic stainless steel), Nd-Fe-B alloy (rare earth magnet), Sm-Fe-N alloy (rare earth magnet), Al-Ni-Co alloy (Alnico magnet) and ferrite. The ferrite may be, for example, spinel ferrite, hexagonal ferrite, or garnet ferrite. The metal element-containing powder may be a copper alloy such as a Cu-Sn alloy, a Cu-Sn-P alloy, a Cu-Ni alloy, or a Cu-Be alloy. The metal element-containing powder may contain one of the above elements and compositions, or may contain a plurality of the above elements and compositions.

[0088] The metal element-containing powder may be Fe simple substance. The metal element-containing powder may be an alloy containing iron (Fe-based alloy). The Fe-based alloy may be, for example, an Fe-Si-Cr-based alloy or an Nd-Fe-B-based alloy. The metal element-containing powder may be at least one of an amorphous iron powder and a carbonyl iron powder. When the metal element-containing powder contains at least one of Fe simple substance and an Fe-based alloy, it is easy to produce a compact having a high space factor and excellent magnetic properties from the compound. The metal element-containing powder may be an Fe amorphous alloy. As a commercially available product of Fe amorphous alloy powder, for example, at least one selected from the group consisting of AW2-08, KUAMET-6B2, KUAMET 9A4-II (all of which are product names manufactured by Epson Atmix Corporation), DAP MS3, DAP MS7, DAP MSA10, DAP PB, DAP PC, DAP MKV49, DAP 410L, DAP 430L, DAP HYB series (all of which are product names manufactured by Daido Steel Co., Ltd.), MH45D, MH28D, MH25D, and MH20D (all of which are product names manufactured by Kobe Steel, Ltd.) may be used.

[0089] <Compound manufacturing method> In the manufacture of the compound, the metal element-containing powder and the resin composition (each component constituting the resin composition) are mixed while being heated. For example, the metal element-containing powder and the resin composition may be kneaded with a kneader, roll, stirrer, etc. while being heated. By heating and mixing the metal element-containing powder and the resin composition, the resin composition adheres to a part or the whole of the surface of the metal element-containing particles constituting the metal element-containing powder to cover the metal element-containing particles, and a part or the whole of the epoxy resin in the resin composition becomes a semi-cured product. As a result, a compound is obtained. The compound may be obtained by further adding wax to the powder obtained by heating and mixing the metal element-containing powder and the resin composition. The resin composition and the wax may be mixed in advance.

[0090] In the kneading, the metal element-containing powder, the siloxane compound, the epoxy resin, the curing agent such as the phenol resin, the curing accelerator, and the coupling agent may be kneaded in the tank. After the metal element-containing powder, the siloxane compound, and the coupling agent are put into the tank and mixed, the epoxy resin, the curing agent, and the curing accelerator may be put into the tank to knead the raw materials in the tank. After the siloxane compound, the epoxy resin, the curing agent, and the coupling agent are kneaded in the tank, the curing accelerator may be put into the tank to further knead the raw materials in the tank. A mixed powder (resin mixed powder) of the epoxy resin, the curing agent, and the curing accelerator may be prepared in advance, and then the metal element-containing powder, the siloxane compound, and the coupling agent are kneaded to prepare a metal mixed powder, and then the metal mixed powder and the above-mentioned resin mixed powder may be kneaded.

[0091] The kneading time depends on the type of kneading machine, the volume of the kneading machine, and the amount of compound produced, but is preferably 1 minute or more, more preferably 2 minutes or more, and even more preferably 3 minutes or more. The kneading time is preferably 20 minutes or less, more preferably 15 minutes or less, and even more preferably 10 minutes or less. If the kneading time is less than 1 minute, the kneading is insufficient, the moldability of the compound is impaired, and the degree of hardening of the compound varies. If the kneading time exceeds 20 minutes, for example, the hardening of the resin composition (e.g., epoxy resin and phenolic resin) proceeds in the tank, and the fluidity and moldability of the compound are likely to be impaired. When the raw materials in the tank are kneaded with a kneader while being heated, the heating temperature may be, for example, a temperature at which a semi-cured product of the epoxy resin (epoxy resin in B stage) is generated and the generation of a hardened product of the epoxy resin (epoxy resin in C stage) is suppressed. The heating temperature may be a temperature lower than the activation temperature of the curing accelerator. The heating temperature is, for example, preferably 50° C. or higher, more preferably 60° C. or higher, and even more preferably 70° C. or higher. The heating temperature is preferably 150° C. or lower, more preferably 120° C. or lower, and even more preferably 110° C. or lower. When the heating temperature is within the above range, the resin composition in the tank softens and tends to coat the surfaces of the metal element-containing particles constituting the metal element-containing powder, a semi-cured epoxy resin is likely to be produced, and complete curing of the epoxy resin during kneading is likely to be suppressed.

[0092] <Molded body> The molded article according to the present embodiment may include the above-mentioned compound. The molded article may include at least one selected from the group consisting of an uncured resin composition, a semi-cured product of the resin composition (a B-stage resin composition), and a cured product of the resin composition (a C-stage resin composition). The molded article may be a cured product of the above-mentioned compound.

[0093] <Method of manufacturing molded body> The method for producing a molded body according to the present embodiment may include a step of pressurizing the compound in a mold. The method for producing a molded body may include only a step of pressurizing the compound in a mold, or may include other steps in addition to the step. The method for producing a molded body may include a first step, a second step, and a third step. Each step will be described in detail below.

[0094] In the first step, a compound is prepared by the method described above.

[0095] In the second step, the compound is pressed in a mold to obtain a molded body (B-stage molded body). Here, the resin composition is filled between the individual metal element-containing particles that make up the metal element-containing powder. The resin composition functions as a binding material (binder) to bind the metal element-containing particles together.

[0096] In the second step, transfer molding of the compound may be performed. In the transfer molding, the compound may be pressurized at 5 MPa or more and 50 MPa or less. The higher the molding pressure, the easier it is to obtain a molded body with excellent mechanical strength. In consideration of the mass productivity of the molded body and the life of the mold, the molding pressure is preferably 8 MPa or more and 20 MPa or less. The density of the molded body formed by transfer molding may be preferably 75% or more and 86% or less, more preferably 80% or more and 86% or less, based on the true density of the compound. When the density of the molded body is 75% or more and 86% or less, a molded body with excellent mechanical strength is easily obtained. In the transfer molding, the second step and the third step may be performed at the same time.

[0097] In the third step, the molded body is cured by heat treatment to obtain a molded body in the C stage. Since the compound according to this embodiment contains a siloxane compound, which is a type of elastomer, the elasticity of the entire compound is reduced, and the stress acting on the compound due to molding shrinkage (thermal curing) of the compound is reduced. As a result, in the process of forming a molded body by thermal curing of the compound, the mold shrinkage rate of the compound is reduced. In addition, although the mechanism is not clear as described above, since the compound according to this embodiment contains a predetermined amount of a siloxane compound, which is a type of elastomer, the heat resistance and voltage resistance of the molded body obtained from the compound are improved. The temperature of the heat treatment may be any temperature at which the resin composition in the molded body is sufficiently cured. The temperature of the heat treatment may be preferably 100°C or more and 300°C or less, more preferably 110°C or more and 250°C or less. In order to suppress oxidation of the metal element-containing powder in the molded body, it is preferable to perform the heat treatment under an inert atmosphere. If the heat treatment temperature exceeds 300° C., the metal element-containing powder may be oxidized or the cured resin may be deteriorated due to a small amount of oxygen inevitably contained in the heat treatment atmosphere. In order to sufficiently cure the resin composition while suppressing the oxidation of the metal element-containing powder and the deterioration of the cured resin, the heat treatment temperature may be maintained for a period of time preferably from several minutes to 10 hours, more preferably from 3 minutes to 8 hours. EXAMPLES

[0098] The present invention will be described in more detail below with reference to examples and comparative examples, but the present invention is not limited to these examples in any way.

[0099] Example 1 [Preparation of compound] 50g of biphenylene aralkyl type epoxy resin, 50g of multifunctional type epoxy resin, 14.5g of phenol novolac resin 1 (hardener), 23.6g of phenol novolac resin 2 (hardener), 5.9g of urea catalyst (hardening accelerator), 7.5g of zinc claurate type metal soap (mold release agent), 2.0g of montanic acid ester (mold release agent (wax)), and 4.0g of natural wax (mold release agent (wax)) were put into a plastic container. These raw materials were mixed in the plastic container for 10 minutes to prepare a resin mixture. The resin mixture corresponds to all other components of the resin composition except for the siloxane compound and the coupling agent. As the biphenylene aralkyl type epoxy resin, NC-3000 manufactured by Nippon Kayaku Co., Ltd. was used. As the multifunctional epoxy resin, VG-3101L manufactured by Printec Co., Ltd. was used. As the phenol novolac resin 1, HF-3M manufactured by Meiwa Kasei Co., Ltd. was used. As the phenol novolac resin 2, MEW-1800 manufactured by Meiwa Kasei Co., Ltd. was used. As the urea-based catalyst, U-CAT3512T manufactured by San-Apro Ltd. was used. As the zinc clawrate type metal soap, Powder Base L manufactured by NOF Corporation was used. As the montanic acid ester, LICOWAX-OP manufactured by Clariant Chemicals Co., Ltd. was used. As the natural wax, Carnauba Wax No. 1 manufactured by Cerarica NODA Co., Ltd. was used.

[0100] Amorphous iron powder 1 and amorphous iron powder 2 were mixed uniformly for 5 minutes in a pressurized twin-shaft kneader (manufactured by Nippon Spindle Manufacturing Co., Ltd., capacity 5 L) to prepare 3741 g of metal element-containing powder. The content of amorphous iron powder 1 in the metal element-containing powder was 82 mass%. The content of amorphous iron powder 2 in the metal element-containing powder was 18 mass%. 1.9 g of methacryloxyoctyltrimethoxysilane (coupling agent), 1.9 g of 3-mercaptopropyltrimethoxysilane (coupling agent), and 15 g of caprolactone-modified dimethyl silicone (compound having a siloxane bond) were added to the metal element-containing powder in the twin-shaft kneader. Next, the contents of the twin-shaft kneader were heated to 90°C, and the contents of the twin-shaft kneader were mixed for 10 minutes while maintaining the temperature. Next, the resin mixture was added to the contents of the twin-screw kneader, and the contents were melted and kneaded for 15 minutes while maintaining the temperature of the contents at 120°C. The kneaded product obtained by the above melting and kneading was cooled to room temperature, and then crushed with a hammer until the kneaded product had a predetermined particle size. Note that the above "melting" means melting at least a part of the resin composition in the contents of the twin-screw kneader. The metal element-containing powder in the compound does not melt during the compound preparation process. As the amorphous iron powder 1, KUAMET 9A4-II 053C03 (average particle size 24 μm) manufactured by Epson Atmix Corporation was used. As the amorphous iron powder 2, AW2-08 (average particle size 5.3 μm) manufactured by Epson Atmix Corporation was used. As methacryloxyoctyltrimethoxysilane, KBM-5803 manufactured by Shin-Etsu Chemical Co., Ltd. was used. As the 3-mercaptopropyltrimethoxysilane, KBM-803 manufactured by Shin-Etsu Chemical Co., Ltd. was used. The caprolactone-modified dimethyl silicone used was DBL-C32 manufactured by Gelest Co., Ltd. This caprolactone-modified dimethyl silicone is a compound represented by the above chemical formula (3).

[0101] By the above method, the compound of Example 1 was prepared. The content of the metal element-containing powder in the compound was 95.5 mass %.

[0102] Other Examples and Comparative Examples Compounds of other examples and comparative examples were prepared in the same manner as in Example 1, except that the raw material formulation was changed as shown in Table 1. Evaluations of the compounds of each example were carried out in the same manner as in Example 1. Note that KBM-403 listed in Table 1 is 3-glycidoxypropyltrimethoxysilane manufactured by Shin-Etsu Chemical Co., Ltd.

[0103] [evaluation] The compounds of the examples and comparative examples were subjected to the following evaluations, and the results are shown in Table 1.

[0104] (Heat resistance evaluation: 250℃ bending test) The compounds of each Example and Comparative Example were transfer molded under the conditions of a mold temperature of 175°C, a molding pressure of 13.5 MPa, and a curing time of 360 seconds, and then post-cured at 175°C for 5.5 hours to obtain test specimens. The dimensions of the test specimens were 80 mm long x 10 mm wide x 3.0 mm thick. A three-point support bending test was carried out on the test specimen using an autograph equipped with a thermostatic chamber. The autograph used was an AGS-500A manufactured by Shimadzu Corporation. The temperature of the thermostatic chamber was 250°C. In the bending test, one side of the test specimen was supported by two supports. A load was applied to the center position between the two supports on the other side of the test specimen. The load at which the test specimen broke was measured. The measurement conditions for the bending test were as follows: Distance between two supports Lv: 64.0±0.5mm Head speed: 2.0±0.2mm / min Chart speed: 100mm / min Chart full scale: 490N(50kgf) The bending strength σ (unit: MPa) was calculated based on the following formula (A). The bending modulus E (unit: GPa) was calculated based on the following formula (B). The bending elongation ε (unit: %) was calculated based on the following formula (C). In the formulas below, "P" is the load (unit: N) when the test piece breaks. "Lv" is the distance between the two supports (unit: mm). "W" is the width of the test piece (unit: mm). "t" is the thickness of the test piece (unit: mm). "F / Y" is the gradient of the linear portion of the load-deflection curve (unit: N / mm). "s" is the deflection of the test piece just before it breaks (unit: mm). σ = (3 × P × Lv) / (2 × W × t 2 ) (A) E=[Lv 3 / (4×W×t 3 )]×(F / Y) (B) ε = (600 × s × t) / Lv 2 (C)

[0105] (Evaluation of voltage resistance: voltage resistance test) The compounds of each of the Examples and Comparative Examples were transfer molded under conditions of a mold temperature of 175°C, a molding pressure of 13.5 MPa, and a curing time of 360 seconds, and then post-cured at 175°C for 5.5 hours to prepare test pieces with a thickness of 2.0 mm. For the voltage withstand test, a stainless steel plate connected to a ground wire, a conductive rubber plate, a test piece, and a 10 mm diameter stainless steel electrode connected to a high voltage wire were placed on an insulating plate in that order. The high voltage wire and ground wire were connected to the high voltage output terminal and ground terminal of a high voltage amplifier, respectively. The waveform output of a function generator was input to the high voltage amplifier to generate a test voltage that increased from 0V to a maximum of 2000V at a rate of 10V per second, and applied to the test piece. The voltage was read when the current passing through the test piece exceeded 10mA. Next, stainless steel electrodes were placed at different positions on the test piece, and voltage was applied in the same manner. This was repeated a specified number of times, and the average of the voltage readings was taken as the voltage withstand voltage (dielectric breakdown voltage: V / mm) of the test piece.

[0106] [Table 1] [Industrial Applicability]

[0107] The compound according to the present invention has high industrial value since it can give a molded article having both heat resistance and voltage resistance.

Claims

1. The present invention comprises a metal element-containing powder and a resin composition, The metal element-containing powder is a magnetic powder, The resin composition contains an epoxy resin and a compound having a siloxane bond, the content of the compound having a siloxane bond is 20 parts by mass or less relative to 100 parts by mass of the epoxy resin, The compound having a siloxane bond includes a siloxane compound having a structure represented by the following chemical formulas (1) and (2). 【Chemistry 1】 [In the above chemical formula (1), n ​​is an integer of 2 to 200, and R １ and R ２ Each of them is independently an alkyl group having 1 to 10 carbon atoms, an aryl group having 6 to 10 carbon atoms, an alkoxy group having 1 to 10 carbon atoms, a monovalent organic group having an epoxy group, a monovalent organic group having a carboxy group, or a polyalkylene ether group having 3 to 500 carbon atoms.] 【Chemistry 2】 [In the above chemical formula (2), R 3 is an alkylene group having 1 to 10 carbon atoms.]

2. A compound as described in claim 1, wherein the average particle diameter of the metal element-containing powder is 1 μm or more and 300 μm or less.

3. The siloxane compound includes a compound represented by the following chemical formula (3): A compound according to claim 1 or 2. 【Chemistry 3】 [In the above chemical formula (3), n is an integer of 2 to 200, and m １ and m ２ each independently represents an integer from 1 to 200; R ４ , R ５ , R ６ and R ７ each independently represents an alkyl group having 1 to 10 carbon atoms, an aryl group having 6 to 10 carbon atoms, an alkoxy group having 1 to 10 carbon atoms, a monovalent organic group having an epoxy group, a monovalent organic group having a carboxy group, or a polyalkylene ether group having 3 to 500 carbon atoms; R ８ and R ９ each independently represents an alkylene group having 1 to 10 carbon atoms; R １０ and R １１ Each of them is independently a divalent hydrocarbon group having 1 to 10 carbon atoms which may contain an ether structure.

4. The epoxy resin includes at least one of a biphenylene aralkyl type epoxy resin and an isocyanate-modified epoxy resin. A compound according to any one of claims 1 to 3.

5. The content of the metal element-containing powder is 90% by mass or more and less than 100% by mass. A compound according to any one of claims 1 to 4.

6. A molded body comprising the compound according to any one of claims 1 to 5.

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