WO2021241513A1 - Compound, molded object, and cured object - Google Patents

Compound, molded object, and cured object Download PDF

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Publication number
WO2021241513A1
WO2021241513A1 PCT/JP2021/019652 JP2021019652W WO2021241513A1 WO 2021241513 A1 WO2021241513 A1 WO 2021241513A1 JP 2021019652 W JP2021019652 W JP 2021019652W WO 2021241513 A1 WO2021241513 A1 WO 2021241513A1
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WO
WIPO (PCT)
Prior art keywords
compound
metal powder
epoxy resin
group
resin
Prior art date
Application number
PCT/JP2021/019652
Other languages
French (fr)
Japanese (ja)
Inventor
貴一 稲葉
翔平 山口
Original Assignee
昭和電工マテリアルズ株式会社
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by 昭和電工マテリアルズ株式会社 filed Critical 昭和電工マテリアルズ株式会社
Priority to JP2022526537A priority Critical patent/JPWO2021241513A1/ja
Priority to KR1020227044003A priority patent/KR20230017227A/en
Priority to CN202180030919.3A priority patent/CN115443297A/en
Publication of WO2021241513A1 publication Critical patent/WO2021241513A1/en

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
    • C08G59/02—Polycondensates containing more than one epoxy group per molecule
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/02—Elements
    • C08K3/08—Metals
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K5/00—Use of organic ingredients
    • C08K5/49—Phosphorus-containing compounds
    • C08K5/51—Phosphorus bound to oxygen
    • C08K5/52—Phosphorus bound to oxygen only
    • C08K5/521—Esters of phosphoric acids, e.g. of H3PO4
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F1/00—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/03—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity
    • H01F1/12—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials
    • H01F1/14—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys
    • H01F1/20—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys in the form of particles, e.g. powder
    • H01F1/22—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys in the form of particles, e.g. powder pressed, sintered, or bound together
    • H01F1/24—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys in the form of particles, e.g. powder pressed, sintered, or bound together the particles being insulated
    • H01F1/26—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys in the form of particles, e.g. powder pressed, sintered, or bound together the particles being insulated by macromolecular organic substances

Definitions

  • the present invention relates to a compound, a molded body, and a cured product.
  • the compound containing the metal powder and the resin composition is used as a raw material for various industrial products according to the physical characteristics of the metal powder.
  • the compound is used as a raw material for an inductor, a sealing material, an electromagnetic wave shield (EMI shield), a bond magnet, or the like (see Patent Document 1 below).
  • the compound When manufacturing an industrial product from a compound, the compound is supplied and filled into the mold through a flow path, and parts such as coils are embedded in the compound in the mold.
  • the fluidity of the compound is required in these steps.
  • the content of the metal powder in the compound increases, the fluidity of the compound is significantly reduced and it becomes difficult to fill the mold.
  • the dimensions of the elements mounted on the electronic devices have become smaller. Therefore, when a compound is used for manufacturing a device, it is necessary that the compound flows in a narrow flow path and the compound that has passed through the narrow flow path is uniformly filled in a fine mold.
  • An object of the present invention is to provide a compound having excellent fluidity. It is also an object of the present invention to provide a molded body containing the compound and a cured product of the compound.
  • the compound according to one aspect of the present invention contains a metal powder and a resin composition containing an epoxy resin, a curing agent and a dispersant, and the content of the metal powder is 90% by mass or more and 98% by mass or less.
  • Dispersant comprises phosphate ester.
  • the phosphoric acid ester may have a group represented by -OR (R indicates an organic group having 4 or more carbon atoms).
  • the organic group may be an alkyl group having 4 or more carbon atoms or a group in which an ether bond is inserted into at least a part of carbon-carbon bonds in an alkyl group having 4 or more carbon atoms.
  • the alkyl group and the group in which the ether bond is inserted in at least a part of the carbon-carbon bond in the alkyl group may have a substituent.
  • the content of the dispersant may be 1 part by mass or less with respect to 100 parts by mass of the metal powder.
  • the molded body according to one aspect of the present invention includes the above compound.
  • the cured product according to one aspect of the present invention is a cured product of the above compound.
  • the present invention it is possible to provide a compound having excellent fluidity. Further, according to the present invention, it is possible to provide a molded product containing the compound and a cured product.
  • the compound of the present invention has a low viscosity and excellent fluidity. Therefore, the compound can be filled into the mold with good filling property.
  • the compound according to the present embodiment includes a metal powder and a resin composition.
  • the metal powder may contain, for example, at least one selected from the group consisting of elemental metals, alloys, amorphous powders and metal compounds.
  • the resin composition contains at least an epoxy resin, a curing agent and a dispersant. Dispersants include phosphate esters. In the compound, the metal powder, epoxy resin, curing agent and dispersant are mixed.
  • the resin composition may further contain a curing accelerator, a mold release agent, an additive and the like as other components.
  • the resin composition is a component that can include an epoxy resin, a curing agent, a dispersant, a curing accelerator, a mold release agent, and an additive, and is a component (nonvolatile component) other than an organic solvent and a metal powder. It may be there.
  • the additive is a component of the rest of the resin composition excluding the epoxy resin, the curing agent, the dispersant, the curing accelerator, and the mold release agent. Additives are, for example, coupling agents, siloxane compounds, flame retardants and the like.
  • the compound may be a powder (compound powder).
  • the compound may include a metal powder and a resin composition attached to the surface of each metal particle constituting the metal powder.
  • the resin composition may cover the entire surface of the particles, or may cover only a part of the surface of the particles.
  • the compound may comprise an uncured resin composition and a metal powder.
  • the compound may include a semi-cured product of the resin composition (for example, a B-stage resin composition) and a metal powder.
  • the compound may comprise both an uncured resin composition and a semi-cured resin composition.
  • the compound may consist of a metal powder and a resin composition.
  • the content of the metal powder in the compound is 90% by mass or more and 98% by mass or less.
  • the content of the metal powder in the compound may be preferably 92% by mass or more and 98% by mass or less, 94% by mass or more and 97.5% by mass or less, or 96% by mass or more and 97.5% by mass or less. If the content of the metal powder in the compound containing no dispersant is 90% by mass or more, the fluidity of the compound is significantly reduced.
  • the compound according to this embodiment contains a phosphate ester as a dispersant. As a result, although the content of the metal powder in the compound is 90% by mass or more, the compound according to the present embodiment is superior to the conventional compound in terms of fluidity.
  • the average particle size of the metal powder is not particularly limited, but may be, for example, 1 ⁇ m or more and 300 ⁇ m or less.
  • the average particle size may be measured, for example, by a particle size distribution meter.
  • the shape of the individual metal particles constituting the metal powder is not limited, but may be spherical, flat, prismatic, or needle-shaped, for example.
  • the compound may comprise a plurality of metal powders having different average particle sizes.
  • the molded body and the cured product formed from the compound can be used as various industrial products. Or it can be used as a raw material for them.
  • Industrial products manufactured using the compound may be, for example, automobiles, medical equipment, electronic equipment, electrical equipment, information communication equipment, home appliances, audio equipment, and general industrial equipment.
  • the compound may be used as a raw material for a bonded magnet.
  • the compound when the compound contains a soft magnetic powder such as Fe—Si—Cr based alloy or ferrite as the metal powder, the compound may be used as an inductor (for example, EMI filter) or a raw material for a transformer (for example, a magnetic core).
  • a molded body eg, a sheet formed from the compound may be used as an electromagnetic wave shield.
  • the resin composition has a function as a binder of metal particles constituting the metal powder, and imparts mechanical strength to the molded body and the cured product formed from the compound.
  • the resin composition contained in the compound is filled between the metal particles when the compound is molded at high pressure using a mold, and the particles are bound to each other.
  • the cured product of the resin composition binds the metal particles more firmly to each other, and a molded body and a cured product having excellent mechanical strength can be obtained.
  • the resin composition according to this embodiment contains an epoxy resin as a thermosetting resin, so that the fluidity of the compound can be improved.
  • the epoxy resin may be, for example, a resin having two or more epoxy groups in one molecule.
  • the type of epoxy resin is not particularly limited and can be selected according to the desired properties of the composition and the like.
  • Epoxy resins include, for example, biphenyl type epoxy resin, stillben type epoxy resin, diphenylmethane type epoxy resin, sulfur atom-containing epoxy resin, novolak type epoxy resin, dicyclopentadiene type epoxy resin, salicylaldehyde type epoxy resin, naphthols and phenol.
  • Copolymerization type epoxy resin aralkyl type phenol resin epoxidized product, bisphenol type epoxy resin, epoxy resin containing bisphenol skeleton, alcoholic glycidyl ether type epoxy resin, paraxylylene and / or metaxylylene modified phenol resin glycidyl ether Type epoxy resin, glycidyl ether type epoxy resin of terpene-modified phenol resin, cyclopentadiene type epoxy resin, glycidyl ether type epoxy resin of polycyclic aromatic ring-modified phenol resin, glycidyl ether type epoxy resin of naphthalene ring-containing phenol resin, glycidyl ester type Epoxy resin, glycidyl type or methyl glycidyl type epoxy resin, alicyclic epoxy resin, halogenated phenol novolac type epoxy resin, orthocresol novolac type epoxy resin, hydroquinone type epoxy resin, trimetylol propane type epoxy resin, and
  • the epoxy resins include biphenyl type epoxy resin, orthocresol novolac type epoxy resin, phenol novolac type epoxy resin, bisphenol type epoxy resin, epoxy resin having a bisphenol skeleton, salicylaldehyde novolak type epoxy resin, and naphthol novolac. It may contain at least one selected from the group consisting of type epoxy resins.
  • the epoxy resin may contain at least one selected from the group consisting of biphenylene aralkyl type epoxy resin and orthocresol novolak type epoxy resin.
  • 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 is excellent in fluidity.
  • the crystalline epoxy resin (highly crystalline epoxy resin) may contain, for example, at least one selected from the group consisting of a hydroquinone type epoxy resin, a bisphenol type epoxy resin, a thioether type epoxy resin, and a 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-865, Epicron HP-4032D, Epicron HP-7200L, Epicron HP-7200, Epicron HP-7200H, Epicron HP-7200HH, Epicron HP-7200HH, Epicron HP-4700, Epicron HP-4710, Epicron HP-4770, Epicron HP-5000, Epicron HP-6000, N500P-2, and N500P-10 (above, trade name manufactured by DIC Co., Ltd.), 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, HPEN-502H, EOCN-1020, EOCN-102S, EOCN-103S, EOCN-104S, CER-1020, EPPN-201, BREN-S, BREN-10S (above, trade name manufactured by Nippon Kayaku Co., Ltd.),
  • the resin composition may contain one of the above epoxy resins.
  • the resin composition may contain a plurality of types of epoxy resins among the above.
  • the resin composition may contain an epoxy resin containing a biphenyl skeleton, an orthocresol novolac type epoxy resin, and a polyfunctional epoxy resin containing two or more epoxy groups.
  • the curing agent is classified into a curing agent that cures the epoxy resin in the range of low temperature to room temperature and a heat curing type curing agent that cures the epoxy resin with heating.
  • the curing agent that cures the epoxy resin in the range of low temperature to room temperature is, for example, aliphatic polyamines, polyaminoamides, and polymercaptans.
  • the heat-curable curing agent is, for example, aromatic polyamine, acid anhydride, phenol novolac resin, dicyandiamide (DICY) and the like.
  • the type of the curing agent is not particularly limited and can be selected according to the desired properties of the composition and the like.
  • the curing agent may be preferably a heat-curing type curing agent, more preferably a phenol resin, and further preferably a phenol novolac resin.
  • a phenol novolac resin as a curing agent, it is easy to obtain a cured product of an epoxy resin having a high glass transition point. As a result, the heat resistance and mechanical strength of the molded body are likely to be improved.
  • the phenol resin is, for example, an aralkyl type phenol resin, a dicyclopentadiene type phenol resin, a salicylaldehyde type phenol resin, a novolak type phenol resin, a copolymerized phenol resin of a benzaldehyde type phenol and an aralkyl type phenol, a paraxylylene and / or a metaxylylene modification.
  • the phenol resin may be a copolymer composed of two or more of the above.
  • phenolic resins for example, Tamanol 758 manufactured by Arakawa Chemical Industry Co., Ltd., HP-850N manufactured by Hitachi Kasei Co., Ltd., MEHC-7500-3S manufactured by Meiwa Kasei Co., Ltd., MEHC-7851SS, etc. may be used. good.
  • the phenol novolac resin may be, for example, a resin obtained by condensing or co-condensing phenols and / or naphthols and aldehydes under an acidic catalyst.
  • the phenols constituting the phenol novolak resin may include, 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 novolak resin may contain, for example, at least one selected from the group consisting of ⁇ -naphthol, ⁇ -naphthol and dihydroxynaphthalene.
  • the aldehydes constituting the phenol novolac resin may contain, for example, at least one selected from the group consisting of formaldehyde, acetaldehyde, propionaldehyde, benzaldehyde and salicylaldehyde.
  • 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 contain, for example, at least one selected from the group consisting of resorcin, catechol, bisphenol A, bisphenol F, and substituted or unsubstituted biphenol.
  • the resin composition may contain one of the above phenolic resins.
  • the resin composition may include a plurality of types of phenol resins among the above.
  • the resin composition may contain one of the above-mentioned curing agents.
  • the resin composition may contain a plurality of types of curing agents among the above.
  • the ratio of the active group (phenolic OH group) in the curing agent that reacts with the epoxy group in the epoxy resin is preferably 0.5 to 1.5 equivalents, more preferably 0.5 equivalents, relative to 1 equivalent of the epoxy group in the epoxy resin. May be 0.6 to 1.4 equivalents, more preferably 0.7 to 1.2 equivalents.
  • the ratio of active groups in the curing agent is less than 0.5 equivalent, it is difficult to obtain a sufficient elastic modulus of the obtained cured product.
  • 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.
  • the ratio of the active group in the curing agent is out of the above range, the effect according to the present invention can be obtained.
  • the fluidity of the compound can be improved. This makes it possible to suppress unfilling during molding and generation of voids in the molded body.
  • the reason for the improved fluidity of the compound is not always clear, but the inventors have found that the phosphate groups of the phosphate ester are selectively adsorbed on the metal powder, which improves the dispersibility of the metal powder and thus flows. It is speculated that the sex will improve.
  • the phosphoric acid ester may be either a phosphoric acid monoester, a phosphoric acid diester or a phosphoric acid triester, but from the viewpoint of improving the fluidity of the compound, n in the above formula is 1 or 2. , Phosphoric acid monoester or phosphoric acid diester.
  • the phosphoric acid ester may preferably have a group represented by -OR (R indicates an organic group having 4 or more carbon atoms).
  • R indicates an organic group having 4 or more carbon atoms.
  • the carbon number of R may be 5 or more, and may be 6 or more.
  • the carbon number of R can be 20 or less, and may be 15 or less.
  • the organic group may be an alkyl group having 4 or more carbon atoms or a group in which an ether bond is inserted in at least a part of carbon-carbon bonds in an alkyl group having 4 or more carbon atoms. This makes it easy to improve the fluidity of the compound.
  • the alkyl group may be a linear or branched alkyl group.
  • the alkyl group and the group in which the ether bond is inserted in at least a part of the carbon-carbon bond in the alkyl group may have a substituent (reactive group).
  • the substituent include an amino group, a ureido group, an epoxy group, a thiol group, a (meth) acryloyl group, a hydroxy group and the like.
  • the above-mentioned "carbon number" in the organic group R is a number not including the carbon number contained in the substituent.
  • Examples of commercially available phosphoric acid esters include JP-504, JP-506H, JP-508, and JP-513 manufactured by Johoku Chemical Industry Co., Ltd.
  • the compound 1 represented by the following chemical formula 1 may be, for example, JP-504.
  • the compound 2 represented by the following chemical formula 2 may be, for example, JP-506H described above.
  • the compound 3 represented by the following chemical formula 3 may be, for example, JP-508.
  • the compound 4 represented by the following chemical formula 4 may be, for example, JP-513.
  • N in the above chemical formula 1 may be 1 or 2.
  • N in the above chemical formula 1 may be 1 or more and 3 or less.
  • N in the above chemical formula 2 may be 1 or 2.
  • N in the above chemical formula 2 may be 1 or more and 3 or less.
  • N in the above chemical formula 3 may be 1 or 2.
  • N in the above chemical formula 3 may be 1 or more and 3 or less.
  • (Is в-C 13 H 27 O) n OP (OH) 3-n (4) N in the above chemical formula 4 may be 1 or 2.
  • N in the above chemical formula 4 may be 1 or more and 3 or less.
  • the blending amount of the dispersant is 1 part by mass or less, 0.5 part by mass or less, 0.1 part by mass or less, or 0.05 with respect to 100 parts by mass of the metal powder from the viewpoint of improving the fluidity of the compound. It may be less than or equal to a mass part. From the same viewpoint, the blending amount may be 0.01 parts by mass or more.
  • the curing accelerator is not limited as long as it is a composition that reacts with the epoxy resin to accelerate the curing of the epoxy resin, for example.
  • the curing accelerator may be, for example, a phosphorus-based curing accelerator, an imidazole-based curing accelerator, or a urea-based curing accelerator.
  • the resin composition contains a curing accelerator, the moldability and releasability of the compound can be improved.
  • the resin composition contains a curing accelerator, the mechanical strength of a molded product or a cured product (for example, an electronic component) manufactured by using a compound is improved, or in a high temperature and high humidity environment. The storage stability of the compound is improved.
  • Examples of the phosphorus-based curing accelerator include phosphine compounds and phosphonium salt compounds.
  • imidazole-based curing accelerators include, for example, 2MZ-H, C11Z, C17Z, 1,2DMZ, 2E4MZ, 2PZ-PW, 2P4MZ, 1B2MZ, 1B2PZ, 2MZ-CN, C11Z-CN, 2E4MZ-CN, 2PZ.
  • -At least one selected from the group consisting of CN, C11Z-CNS, 2P4MHZ, TPZ, and SFZ above, trade name manufactured by Shikoku Chemicals Corporation may be used.
  • the urea-based curing accelerator is not particularly limited as long as it is a curing accelerator having a urea group, but from the viewpoint of improving storage stability, an alkyl urea-based curing accelerator having an alkyl urea group is preferable.
  • the alkylurea-based curing accelerator having an alkylurea group include aromatic alkylurea and aliphatic alkylurea.
  • Examples of commercially available alkyl urea-based curing accelerators include U-CAT3512T (trade name, manufactured by San-Apro Co., Ltd., aromatic dimethyl urea) and U-CAT3513N (trade name, manufactured by San-Apro Co., Ltd., aliphatic dimethyl urea). Can be mentioned.
  • aromatic alkylurea is preferable because the cleavage temperature is moderately low and the compound can be easily cured efficiently.
  • the amount of the curing accelerator to be blended is not particularly limited as long as it can obtain the curing promoting effect.
  • the amount of the curing accelerator is preferably 0.1 part by mass or more and 30 parts by mass with respect to 100 parts by mass of the epoxy resin.
  • it may be more preferably 1 part by mass or more and 15 parts by mass or less.
  • the content of the curing accelerator is preferably 0.001 part by mass or more and 5 parts by mass or less with respect to 100 parts by mass of the total mass of the epoxy resin and the phenol resin.
  • the blending amount of the curing accelerator is less than 0.1 parts by mass, it is difficult to obtain a sufficient curing promoting effect.
  • the blending amount of the curing accelerator exceeds 30 parts by mass, the storage stability of the compound tends to decrease. However, even when the blending amount and content of the curing accelerator are out of the above range, the effect according to the present invention can be obtained.
  • the coupling agent improves the adhesion between the resin composition and the metal element-containing particles constituting the metal powder, and improves the flexibility and mechanical strength of the molded product formed from the compound.
  • the coupling agent may be, for example, at least one selected from the group consisting of a silane compound (silane coupling agent), a titanium compound, an aluminum compound (aluminum chelate), and an aluminum / zirconium compound.
  • the silane coupling agent may be at least one selected from the group consisting of, for example, epoxysilane, mercaptosilane, aminosilane, alkylsilane, ureidosilane, acid anhydride-based silane, vinylsilane and (meth) acryloyloxysilane.
  • the resin composition may contain one of the above-mentioned coupling agents, and may contain a plurality of of the above-mentioned coupling agents.
  • the resin composition may contain a compound having a siloxane bond (siloxane compound) because the molding shrinkage rate of the compound is easily reduced and the heat resistance and withstand voltage resistance of the molded product are easily improved.
  • 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 compound may contain flame retardants due to the environmental safety, recyclability, moldability and low cost of the compound.
  • the flame retardant is at least selected from the group consisting of, for example, a bromine-based flame retardant, a phosphorus-based flame retardant, a hydrated metal compound-based flame retardant, a silicone-based flame retardant, a nitrogen-containing compound, a hindered amine compound, an organic metal compound, and an aromatic empra. It may be a kind.
  • the resin composition may contain one of the above flame retardants, and may contain a plurality of of the above flame retardants.
  • the resin composition may contain a mold release agent.
  • the mold release agent also functions as an agent for improving the fluidity of the compound in the molding of the compound (for example, transfer molding).
  • the release agent include fatty acids such as higher fatty acids, fatty acid esters, and fatty acid metal salts.
  • the release agent is, for example, fatty acids such as montanic acid, stearic acid, 12-oxystearic acid, lauric acid or esters thereof (for example, alkyl esters); zinc stearate, calcium stearate, barium steaenoate, aluminum stearate, etc.
  • fatty acids such as montanic acid, stearic acid, 12-oxystearic acid, lauric acid or esters thereof (for example, alkyl esters); zinc stearate, calcium stearate, barium steaenoate, aluminum stearate, etc.
  • Fatty acid salts such as magnesium stearate, calcium laurate, zinc linoleate, calcium lysinolate, zinc 2-ethylhexoneate; stearic acid amide, oleate amide, erucic acid amide, behenic acid amide, palmitate amide, lauric acid amide, hydroxy Stearic acid amide, methylene bisstearic acid amide, ethylene bisstearic acid amide, ethylene bislauric acid amide, distealyl adipic acid amide, ethylene bisoleic acid amide, diorail adipic acid amide, N-stearyl stearic acid amide, N-oleyl Stearic acid amides, N-stearyl erucate amides, methylol stearic acid amides, methylol behenic acid amides and other fatty acid amides; alcohols such as ethylene glycol and stearyl alcohol; polyethylene glycols, poly
  • Polyethers consisting of; fluorine compounds such as fluorine oil, fluorine grease, and fluorine-containing resin powder; and waxes such as paraffin wax, polyethylene wax, amido wax, polypropylene wax, ester wax, carnauba, and microwax; It may be at least one selected from the group of
  • the metal powder may contain, for example, at least one selected from the group consisting of elemental metals, alloys and metal compounds.
  • the metal powder may consist of, for example, at least one selected from the group consisting of elemental metals, alloys and metal compounds.
  • the alloy may contain at least one selected from the group consisting of solid solutions, eutectic and intermetallic compounds.
  • the alloy may be, for example, stainless steel (Fe—Cr based alloy, Fe—Ni—Cr based alloy, etc.).
  • the metal compound may be, for example, an oxide such as ferrite.
  • the metal powder may contain one kind of metal element or a plurality of kinds of metal elements.
  • the metal element contained in the metal powder may be, for example, a base metal element, a noble metal element, a transition metal element, or a rare earth element.
  • the compound may contain one kind of metal powder, and may contain a plurality of kinds of metal powder having different compositions.
  • the metal powder is not limited to the above composition.
  • the metal elements contained in the metal powder are, for example, iron (Fe), copper (Cu), titanium (Ti), manganese (Mn), cobalt (Co), nickel (Ni), zinc (Zn), and aluminum (Al).
  • Tin (Sn) Chromium (Cr), Niob (Nb), Barium (Ba), Strontium (Sr), Lead (Pb), Silver (Ag), Placeodim (Pr), Neodim (Nd), Samalium (Sm) And at least one selected from the group consisting of dysprosium (Dy).
  • the metal powder may further contain an element other than the metal element.
  • the metal powder may contain, for example, carbon (C), oxygen ( ⁇ ), beryllium (Be), phosphorus (P), sulfur (S), boron (B), or silicon (Si).
  • the metal powder may be a magnetic powder.
  • the metal powder may be a soft magnetic alloy or a ferromagnetic alloy.
  • the metal powder is, for example, Fe-Si alloy, Fe—Si—Al alloy (Sendust), Fe—Ni alloy (Permalloy), Fe—Cu—Ni alloy (Permalloy), Fe—Co alloy (Permalloy). Menzur), 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 (Arnico) It may be a magnetic powder consisting of at least one selected from the group consisting of (magnet) and ferrite.
  • the ferrite may be, for example, spinel ferrite, hexagonal ferrite, or garnet ferrite.
  • the metal powder may be a copper alloy such as a Cu—Sn based alloy, a Cu—Sn—P based alloy, a Cu—Ni based alloy, or a Cu—Be based alloy.
  • the metal powder may contain one of the above elements and compositions, and may contain a plurality of of the above elements and compositions.
  • the metal powder may be Fe alone.
  • the metal powder may be an alloy containing iron (Fe-based alloy).
  • the Fe-based alloy may be, for example, a Fe—Si—Cr based alloy or an Nd—Fe—B based alloy.
  • the metal powder may be at least one of amorphous iron powder and carbonyl iron powder. When the metal powder contains at least one of Fe simple substance and Fe-based alloy, it is easy to produce a molded product having a high space factor and excellent magnetic properties from the compound.
  • the metal powder may be an Fe amorphous alloy.
  • Fe amorphous alloy powders include, for example, AW2-08, KUAMET-6B2, 9A4-II (above, trade name manufactured by Epson Atmix Co., Ltd.), DAP MS3, DAP MS7, DAP MSA10, DAP PB, DAP. Consists of PC, DAP MKV49, DAP 410L, DAP 430L, DAP HYB series (above, product name manufactured by Daido Special Steel Co., Ltd.), MH45D, MH28D, MH25D, and MH20D (above, product name manufactured by Kobe Steel Co., Ltd.). At least one selected from the group may be used.
  • the compound is produced by mixing the metal powder and the resin composition (each component constituting the resin composition) while heating.
  • the metal powder and the resin composition may be kneaded with a kneader, a roll, a stirrer, or the like while heating.
  • the resin composition adheres to a part or the whole of the surface of the metal element-containing particles constituting the metal powder to cover the metal element-containing particles, and the epoxy in the resin composition.
  • Part or all of the resin becomes a semi-cured product.
  • a compound may be obtained by further adding wax to the powder obtained by heating and mixing the metal powder and the resin composition.
  • the resin composition and the wax may be mixed in advance.
  • metal powder, epoxy resin, curing agent, dispersant, curing accelerator and coupling agent may be kneaded in the tank.
  • the epoxy resin, the curing agent and the curing accelerator may be put into the tank and the raw materials in the tank may be kneaded.
  • the curing accelerator may be put in the tank and the raw materials in the tank may be further kneaded.
  • a mixture (resin mixture) of an epoxy resin, a curing agent, a curing accelerator and a dispersant is prepared in advance, and then a metal powder and a coupling agent are kneaded to prepare a metal mixture, and then a metal mixture is prepared. You may knead with the above resin mixture.
  • a mold release agent it may be blended at the same timing as the dispersant.
  • a siloxane compound When a siloxane compound is used, it may be blended at the same timing as the coupling agent.
  • the kneading time depends on the type of the kneading machine, the volume of the kneading machine, and the production amount of the compound, but for example, it is preferably 1 minute or more, more preferably 2 minutes or more, and 3 minutes or more. Is more preferable.
  • the kneading time is preferably 20 minutes or less, more preferably 15 minutes or less, and even more preferably 10 minutes or less. When the kneading time is less than 1 minute, the kneading is insufficient, the moldability of the compound is impaired, and the degree of curing of the compound tends to vary.
  • the resin composition for example, epoxy resin and curing agent
  • the heating temperature is, for example, a semi-cured epoxy resin (B-stage epoxy resin) and a cured epoxy resin (C-stage epoxy resin). It suffices as long as it is a temperature at which the formation of the epoxy is suppressed.
  • the heating temperature may be lower than the activation temperature of the curing accelerator.
  • the heating temperature is, for example, preferably 50 ° C. or higher, more preferably 60 ° C.
  • the heating temperature is preferably 150 ° C. or lower, more preferably 120 ° C. or lower, and even more preferably 110 ° C. or lower.
  • the resin composition in the tank softens and easily covers the surface of the metal element-containing particles constituting the metal powder, and a semi-cured epoxy resin is easily produced, and is being kneaded. Complete curing of the epoxy resin is likely to be suppressed.
  • the molded body according to the present embodiment may be provided with the above-mentioned compound.
  • the cured product according to the present embodiment is obtained by curing the above-mentioned compound, and may be contained in the above-mentioned molded body.
  • the molded body is at least one selected from the group consisting of an uncured resin composition, a semi-cured resin composition (B-stage resin composition), and a cured resin composition (C-stage resin composition). May include.
  • the molded body according to the present embodiment may be used as a sealing material for an electronic component or an electronic circuit board. Thereby, it is possible to suppress cracks in the molded body due to the difference in the coefficient of thermal expansion between the metal member included in the electronic component or the electronic circuit board and the molded body (sealing material).
  • the molded body is manufactured by a manufacturing method including a step of pressurizing the compound in a mold.
  • the method for producing a molded body may include a step of pressurizing a compound covering a part or the whole of the surface of a metal member in a mold.
  • the method for producing the molded body may include only the step of pressurizing the compound in the mold, and may include other steps in addition to the step.
  • the method for producing the molded body may include a first step, a second step, and a third step. Hereinafter, the details of each step will be described.
  • the compound is prepared by the above method.
  • a molded body (B stage molded body) is obtained by pressurizing the compound in the mold.
  • a molded body (B stage molded body) may be obtained by pressing a compound covering a part or the whole of the surface of the metal member in the mold.
  • the resin composition is filled between the individual metal element-containing particles constituting the metal powder. The resin composition then functions as a binder and binds the metal element-containing particles to each other.
  • transfer molding of the compound may be carried out.
  • the compound may be pressurized at 3 MPa or more and 50 MPa or less.
  • the higher the molding pressure the easier it is to obtain a molded body having excellent mechanical strength.
  • the molding pressure is preferably 8 MPa or more and 20 MPa or less.
  • the density of the molded product formed by transfer molding may be preferably 75% or more and 86% or less, and more preferably 80% or more and 86% or less with respect to the true density of the compound. When the density of the molded body is 75% or more and 86% or less, it is easy to obtain a molded body having excellent mechanical strength.
  • the second step and the third step may be carried out collectively.
  • the molded body is cured by heat treatment to obtain a C-stage molded body.
  • the temperature of the heat treatment may be any temperature as long as the resin composition in the molded body is sufficiently cured.
  • the temperature of the heat treatment may be preferably 100 ° C. or higher and 300 ° C. or lower, and more preferably 110 ° C. or higher and 250 ° C. or lower.
  • the heat treatment temperature exceeds 300 ° C., the metal powder is oxidized or the cured resin product is deteriorated by a small amount of oxygen inevitably contained in the heat treatment atmosphere.
  • the heat treatment temperature holding time is preferably several minutes or more and 10 hours or less, more preferably 3 minutes or more 8 It may be less than an hour.
  • the following phosphoric acid ester having a group represented by "-OR" ⁇ R is an organic group having 4 carbon atoms (trade name: JP-504 manufactured by Johoku Chemical Industry Co., Ltd.) -Phosphoric acid ester in which R is an organic group having 6 carbon atoms (trade name: JP-506H manufactured by Johoku Chemical Industry Co., Ltd.) -Phosphoric acid ester in which R is an organic group having 8 carbon atoms (trade name: JP-508 manufactured by Johoku Chemical Industry Co., Ltd.) -Phosphoric acid ester in which R is an organic group having 13 carbon atoms (trade name: JP-513 manufactured by Johoku Chemical Industry Co., Ltd.)
  • Amorphous iron powder (trade name: 9A4-II manufactured by Epson Atmix Co., Ltd., average particle size 24 ⁇ m)
  • Amorphous iron powder (trade name: AW2-08, average particle size 5.3 ⁇ m manufactured by Epson Atmix Co., Ltd.)
  • the two types of amorphous iron powder shown in Table 1 were uniformly mixed for 5 minutes with a pressurized twin-screw kneader (manufactured by Nihon Spindle Manufacturing Co., Ltd., capacity 5 L) to prepare a metal powder.
  • the coupling agent shown in Table 1 and the siloxane compound were added to the metal powder in the biaxial kneader.
  • the contents of the twin-screw kneader were heated to 90 ° C., and the contents of the twin-screw kneader were mixed for 10 minutes while maintaining the temperature.
  • the above 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 was crushed with a hammer until the kneaded product had a predetermined particle size.
  • the above-mentioned "melting” means melting at least a part of the resin composition in the contents of the twin-screw kneader.
  • the metal powder in the compound does not melt during the compound preparation process.
  • the compound of the example was prepared by the above method.
  • the compound of the comparative example was prepared by operating in the same manner as in the examples except that the compounding amount of the metal powder was changed as shown in Table 1 without using the dispersant.

Abstract

A compound which comprises a metal powder and a resin composition comprising an epoxy resin, a hardener, and a dispersant, wherein the content of the metal powder is 90-98 mass% and the dispersant comprises a phosphoric acid ester.

Description

コンパウンド、成型体、及び硬化物Compounds, moldings, and hardened materials
　本発明は、コンパウンド、成型体、及び硬化物に関する。 The present invention relates to a compound, a molded body, and a cured product.
　金属粉末及び樹脂組成物を含むコンパウンドは、金属粉末の諸物性に応じて、多様な工業製品の原材料として利用される。例えば、コンパウンドは、インダクタ、封止材、電磁波シールド（ＥＭＩシールド）、又はボンド磁石等の原材料として利用される（下記特許文献１参照。）。 The compound containing the metal powder and the resin composition is used as a raw material for various industrial products according to the physical characteristics of the metal powder. For example, the compound is used as a raw material for an inductor, a sealing material, an electromagnetic wave shield (EMI shield), a bond magnet, or the like (see Patent Document 1 below).
特開２０１４－１３８０３号公報Japanese Unexamined Patent Publication No. 2014-13803
　コンパウンドから工業製品を製造する場合、流路を通じてコンパウンドを型内へ供給及び充填したり、コイル等の部品を型内のコンパウンド中に埋め込んだりする。これらの工程ではコンパウンドの流動性が要求される。しかしながら、コンパウンド中の金属粉の含有量が多くなってくると、コンパウンドの流動性が顕著に低減し、また型内へ充填され難くなる。近年の電子機器の小型化に伴って、電子機器に搭載される素子の寸法は小さくなっている。したがって、素子の製造にコンパウンドを用いる場合、コンパウンドが狭い流路内で流動し、狭い流路を経たコンパウンドが微細な型内へ均一に充填されることが必要である。 When manufacturing an industrial product from a compound, the compound is supplied and filled into the mold through a flow path, and parts such as coils are embedded in the compound in the mold. The fluidity of the compound is required in these steps. However, as the content of the metal powder in the compound increases, the fluidity of the compound is significantly reduced and it becomes difficult to fill the mold. With the recent miniaturization of electronic devices, the dimensions of the elements mounted on the electronic devices have become smaller. Therefore, when a compound is used for manufacturing a device, it is necessary that the compound flows in a narrow flow path and the compound that has passed through the narrow flow path is uniformly filled in a fine mold.
　本発明は、流動性に優れるコンパウンドを提供することを目的とする。本発明はまた、当該コンパウンドを含む成型体、及びコンパウンドの硬化物を提供することを目的とする。 An object of the present invention is to provide a compound having excellent fluidity. It is also an object of the present invention to provide a molded body containing the compound and a cured product of the compound.
　本発明の一側面に係るコンパウンドは、金属粉と、エポキシ樹脂、硬化剤及び分散剤を含有する樹脂組成物と、を含み、金属粉の含有量が、９０質量％以上９８質量％以下であり、分散剤が、リン酸エステルを含む。 The compound according to one aspect of the present invention contains a metal powder and a resin composition containing an epoxy resin, a curing agent and a dispersant, and the content of the metal powder is 90% by mass or more and 98% by mass or less. , Dispersant comprises phosphate ester.
　一態様において、リン酸エステルが、－ＯＲ（Ｒは炭素数４以上の有機基を示す）で表される基を有してよい。 In one embodiment, the phosphoric acid ester may have a group represented by -OR (R indicates an organic group having 4 or more carbon atoms).
　一態様において、有機基が、炭素数４以上のアルキル基、又は炭素数４以上のアルキル基中の炭素－炭素結合の少なくとも一部にエーテル結合が挿入された基であってよい。 In one embodiment, the organic group may be an alkyl group having 4 or more carbon atoms or a group in which an ether bond is inserted into at least a part of carbon-carbon bonds in an alkyl group having 4 or more carbon atoms.
　一態様において、アルキル基、及びアルキル基中の炭素－炭素結合の少なくとも一部にエーテル結合が挿入された基が置換基を有してよい。 In one embodiment, the alkyl group and the group in which the ether bond is inserted in at least a part of the carbon-carbon bond in the alkyl group may have a substituent.
　一態様において、分散剤の含有量が、金属粉１００質量部に対して１質量部以下であってよい。 In one embodiment, the content of the dispersant may be 1 part by mass or less with respect to 100 parts by mass of the metal powder.
　本発明の一側面に係る成型体は、上記コンパウンドを含む。 The molded body according to one aspect of the present invention includes the above compound.
　本発明の一側面に係る硬化物は、上記コンパウンドの硬化物である。 The cured product according to one aspect of the present invention is a cured product of the above compound.
　本発明によれば、流動性に優れるコンパウンドを提供することができる。また、本発明によれば、当該コンパウンドを含む成型体、及び硬化物を提供することができる。本発明のコンパウンドは低粘度であり優れた流動性を有する。したがって、充填性良くコンパウンドを型内へ充填することができる。 According to the present invention, it is possible to provide a compound having excellent fluidity. Further, according to the present invention, it is possible to provide a molded product containing the compound and a cured product. The compound of the present invention has a low viscosity and excellent fluidity. Therefore, the compound can be filled into the mold with good filling property.
　以下、本発明の好適な実施形態について説明する。ただし、本発明は下記実施形態に何ら限定されるものではない。 Hereinafter, preferred embodiments of the present invention will be described. However, the present invention is not limited to the following embodiments.
［コンパウンド］
　本実施形態に係るコンパウンドは、金属粉と、樹脂組成物と、を備える。金属粉は、例えば、金属単体、合金、アモルファス粉及び金属化合物からなる群より選ばれる少なくとも一種を含有してよい。樹脂組成物は、少なくともエポキシ樹脂、硬化剤及び分散剤を含有する。分散剤は、リン酸エステルを含む。コンパウンドにおいて、金属粉、エポキシ樹脂、硬化剤及び分散剤は混合されている。樹脂組成物は、他の成分として硬化促進剤、離型剤、添加剤等を更に含有してよい。樹脂組成物は、エポキシ樹脂、硬化剤、分散剤、硬化促進剤、離型剤及び添加剤を包含し得る成分であって、有機溶媒と金属粉とを除く残りの成分（不揮発性成分）であってよい。添加剤とは、樹脂組成物のうち、エポキシ樹脂、硬化剤、分散剤、硬化促進剤及び離型剤を除く残部の成分である。添加剤は、例えば、カップリング剤、シロキサン化合物、難燃剤等である。コンパウンドは、粉末（コンパウンド粉）であってよい。 [compound]
The compound according to the present embodiment includes a metal powder and a resin composition. The metal powder may contain, for example, at least one selected from the group consisting of elemental metals, alloys, amorphous powders and metal compounds. The resin composition contains at least an epoxy resin, a curing agent and a dispersant. Dispersants include phosphate esters. In the compound, the metal powder, epoxy resin, curing agent and dispersant are mixed. The resin composition may further contain a curing accelerator, a mold release agent, an additive and the like as other components. The resin composition is a component that can include an epoxy resin, a curing agent, a dispersant, a curing accelerator, a mold release agent, and an additive, and is a component (nonvolatile component) other than an organic solvent and a metal powder. It may be there. The additive is a component of the rest of the resin composition excluding the epoxy resin, the curing agent, the dispersant, the curing accelerator, and the mold release agent. Additives are, for example, coupling agents, siloxane compounds, flame retardants and the like. The compound may be a powder (compound powder).
　コンパウンドは、金属粉と、当該金属粉を構成する個々の金属粒子の表面に付着した樹脂組成物と、を備えてよい。樹脂組成物は、当該粒子の表面の全体を覆っていてもよく、当該粒子の表面の一部のみを覆っていてもよい。コンパウンドは、未硬化の樹脂組成物と金属粉とを備えてよい。コンパウンドは、樹脂組成物の半硬化物（例えばＢステージの樹脂組成物）と金属粉とを備えてよい。コンパウンドは、未硬化の樹脂組成物、及び樹脂組成物の半硬化物の両方を備えてもよい。コンパウンドは、金属粉と樹脂組成物とからなっていてよい。 The compound may include a metal powder and a resin composition attached to the surface of each metal particle constituting the metal powder. The resin composition may cover the entire surface of the particles, or may cover only a part of the surface of the particles. The compound may comprise an uncured resin composition and a metal powder. The compound may include a semi-cured product of the resin composition (for example, a B-stage resin composition) and a metal powder. The compound may comprise both an uncured resin composition and a semi-cured resin composition. The compound may consist of a metal powder and a resin composition.
　コンパウンド中の金属粉の含有量は、９０質量％以上９８質量％以下である。コンパウンド中の金属粉の含有量は、好ましくは、９２質量％以上９８質量％以下、９４質量％以上９７．５質量％以下、又は９６質量％以上９７．５質量％以下であってよい。仮に分散剤を含まないコンパウンド中の金属粉の含有量が９０質量％以上である場合、コンパウンドの流動性は顕著に低減する。一方、本実施形態に係るコンパウンドは、分散剤としてリン酸エステルを含む。その結果、コンパウンド中の金属粉の含有量が９０質量％以上であるにもかかわらず、本実施形態に係るコンパウンドは流動性において従来のコンパウンドよりも優れている。 The content of the metal powder in the compound is 90% by mass or more and 98% by mass or less. The content of the metal powder in the compound may be preferably 92% by mass or more and 98% by mass or less, 94% by mass or more and 97.5% by mass or less, or 96% by mass or more and 97.5% by mass or less. If the content of the metal powder in the compound containing no dispersant is 90% by mass or more, the fluidity of the compound is significantly reduced. On the other hand, the compound according to this embodiment contains a phosphate ester as a dispersant. As a result, although the content of the metal powder in the compound is 90% by mass or more, the compound according to the present embodiment is superior to the conventional compound in terms of fluidity.
　金属粉の平均粒子径は、特に限定されないが、例えば、１μｍ以上３００μｍ以下であってよい。平均粒子径は、例えば粒度分布計によって測定されてよい。金属粉を構成する個々の金属粒子の形状は限定されないが、例えば、球状、扁平形状、角柱状又は針状であってよい。コンパウンドは、平均粒子径が異なる複数種の金属粉を備えてよい。 The average particle size of the metal 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 the individual metal particles constituting the metal powder is not limited, but may be spherical, flat, prismatic, or needle-shaped, for example. The compound may comprise a plurality of metal powders having different average particle sizes.
　コンパウンドに含まれる金属粉の組成又は組合せに応じて、コンパウンドから形成される成型体及び硬化物の電磁気的特性等の諸特性を自在に制御できるため、当該成型体及び硬化物を様々な工業製品又はそれらの原材料に利用することができる。コンパウンドを用いて製造される工業製品は、例えば、自動車、医療機器、電子機器、電気機器、情報通信機器、家電製品、音響機器、及び一般産業機器であってよい。例えば、コンパウンドが金属粉としてＳｍ－Ｆｅ－Ｎ系合金又はＮｄ－Ｆｅ－Ｂ系合金等の永久磁石を含む場合、コンパウンドは、ボンド磁石の原材料として利用されてよい。コンパウンドが金属粉としてＦｅ－Ｓｉ－Ｃｒ系合金又はフェライト等の軟磁性粉を含む場合、コンパウンドは、インダクタ（例えばＥＭＩフィルタ）又はトランスの原材料（例えば磁芯）として利用されてよい。コンパウンドが金属粉として鉄と銅とを含む場合、コンパウンドから形成された成型体（例えばシート）は、電磁波シールドとして利用されてよい。 Since various properties such as the electromagnetic properties of the molded body and the cured product formed from the compound can be freely controlled according to the composition or combination of the metal powder contained in the compound, the molded body and the cured product can be used as various industrial products. Or it can be used as a raw material for them. Industrial products manufactured using the compound may be, for example, automobiles, medical equipment, electronic equipment, electrical equipment, information communication equipment, home appliances, audio equipment, and general industrial equipment. For example, when the compound contains a permanent magnet such as a Sm—Fe—N alloy or an Nd—Fe—B alloy as a metal powder, the compound may be used as a raw material for a bonded magnet. When the compound contains a soft magnetic powder such as Fe—Si—Cr based alloy or ferrite as the metal powder, the compound may be used as an inductor (for example, EMI filter) or a raw material for a transformer (for example, a magnetic core). When the compound contains iron and copper as metal powder, a molded body (eg, a sheet) formed from the compound may be used as an electromagnetic wave shield.
（樹脂組成物）
　樹脂組成物は、金属粉を構成する金属粒子の結合材（バインダ）としての機能を有し、コンパウンドから形成される成型体及び硬化物に機械的強度を付与する。例えば、コンパウンドに含まれる樹脂組成物は、金型を用いてコンパウンドが高圧で成型される際に、金属粒子の間に充填され、当該粒子を互いに結着する。樹脂組成物を硬化させることにより、樹脂組成物の硬化物が金属粒子同士をより強固に結着して、機械的強度に優れた成型体及び硬化物が得られる。 (Resin composition)
The resin composition has a function as a binder of metal particles constituting the metal powder, and imparts mechanical strength to the molded body and the cured product formed from the compound. For example, the resin composition contained in the compound is filled between the metal particles when the compound is molded at high pressure using a mold, and the particles are bound to each other. By curing the resin composition, the cured product of the resin composition binds the metal particles more firmly to each other, and a molded body and a cured product having excellent mechanical strength can be obtained.
　本実施形態に係る樹脂組成物は、熱硬化性樹脂としてエポキシ樹脂を含有することにより、コンパウンドの流動性を向上することができる。エポキシ樹脂は、例えば、１分子中に２個以上のエポキシ基を有する樹脂であってよい。エポキシ樹脂の種類は特に制限されず、組成物の所望の特性等に応じて選択できる。 The resin composition according to this embodiment contains an epoxy resin as a thermosetting resin, so that the fluidity of the compound can be improved. The epoxy resin may be, for example, a resin having two or more epoxy groups in one molecule. The type of epoxy resin is not particularly limited and can be selected according to the desired properties of the composition and the like.
　エポキシ樹脂は、例えば、ビフェニル型エポキシ樹脂、スチルベン型エポキシ樹脂、ジフェニルメタン型エポキシ樹脂、硫黄原子含有型エポキシ樹脂、ノボラック型エポキシ樹脂、ジシクロペンタジエン型エポキシ樹脂、サリチルアルデヒド型エポキシ樹脂、ナフトール類とフェノール類との共重合型エポキシ樹脂、アラルキル型フェノール樹脂のエポキシ化物、ビスフェノール型エポキシ樹脂、ビスフェノール骨格を含有するエポキシ樹脂、アルコール類のグリシジルエーテル型エポキシ樹脂、パラキシリレン及び／又はメタキシリレン変性フェノール樹脂のグリシジルエーテル型エポキシ樹脂、テルペン変性フェノール樹脂のグリシジルエーテル型エポキシ樹脂、シクロペンタジエン型エポキシ樹脂、多環芳香環変性フェノール樹脂のグリシジルエーテル型エポキシ樹脂、ナフタレン環含有フェノール樹脂のグリシジルエーテル型エポキシ樹脂、グリシジルエステル型エポキシ樹脂、グリシジル型又はメチルグリシジル型のエポキシ樹脂、脂環型エポキシ樹脂、ハロゲン化フェノールノボラック型エポキシ樹脂、オルソクレゾールノボラック型エポキシ樹脂、ハイドロキノン型エポキシ樹脂、トリメチロールプロパン型エポキシ樹脂、及びオレフィン結合を過酢酸等の過酸で酸化して得られる線状脂肪族エポキシ樹脂からなる群より選ばれる少なくとも一種を含んでいてよい。 Epoxy resins include, for example, biphenyl type epoxy resin, stillben type epoxy resin, diphenylmethane type epoxy resin, sulfur atom-containing epoxy resin, novolak type epoxy resin, dicyclopentadiene type epoxy resin, salicylaldehyde type epoxy resin, naphthols and phenol. Copolymerization type epoxy resin, aralkyl type phenol resin epoxidized product, bisphenol type epoxy resin, epoxy resin containing bisphenol skeleton, alcoholic glycidyl ether type epoxy resin, paraxylylene and / or metaxylylene modified phenol resin glycidyl ether Type epoxy resin, glycidyl ether type epoxy resin of terpene-modified phenol resin, cyclopentadiene type epoxy resin, glycidyl ether type epoxy resin of polycyclic aromatic ring-modified phenol resin, glycidyl ether type epoxy resin of naphthalene ring-containing phenol resin, glycidyl ester type Epoxy resin, glycidyl type or methyl glycidyl type epoxy resin, alicyclic epoxy resin, halogenated phenol novolac type epoxy resin, orthocresol novolac type epoxy resin, hydroquinone type epoxy resin, trimetylol propane type epoxy resin, and olefin bond It may contain at least one selected from the group consisting of linear aliphatic epoxy resins obtained by oxidation with a peracid such as peracetic acid.
　流動性の観点において、エポキシ樹脂は、ビフェニル型エポキシ樹脂、オルソクレゾールノボラック型エポキシ樹脂、フェノールノボラック型エポキシ樹脂、ビスフェノール型エポキシ樹脂、ビスフェノール骨格を有するエポキシ樹脂、サリチルアルデヒドノボラック型エポキシ樹脂、及びナフトールノボラック型エポキシ樹脂からなる群より選ばれる少なくとも一種を含んでいてよい。 From the viewpoint of fluidity, the epoxy resins include biphenyl type epoxy resin, orthocresol novolac type epoxy resin, phenol novolac type epoxy resin, bisphenol type epoxy resin, epoxy resin having a bisphenol skeleton, salicylaldehyde novolak type epoxy resin, and naphthol novolac. It may contain at least one selected from the group consisting of type epoxy resins.
　機械強度の観点において、エポキシ樹脂は、ビフェニレンアラルキル型エポキシ樹脂及びオルソクレゾールノボラック型エポキシ樹脂からなる群より選ばれる少なくとも一種を含んでいてよい。 From the viewpoint of mechanical strength, the epoxy resin may contain at least one selected from the group consisting of biphenylene aralkyl type epoxy resin and orthocresol novolak type epoxy resin.
　エポキシ樹脂は、結晶性のエポキシ樹脂であってよい。結晶性のエポキシ樹脂の分子量は比較的低いにもかかわらず、結晶性のエポキシ樹脂は比較的高い融点を有し、且つ流動性に優れる。結晶性のエポキシ樹脂（結晶性の高いエポキシ樹脂）は、例えば、ハイドロキノン型エポキシ樹脂、ビスフェノール型エポキシ樹脂、チオエーテル型エポキシ樹脂、及びビフェニル型エポキシ樹脂からなる群より選ばれる少なくとも一種を含んでいてよい。結晶性のエポキシ樹脂の市販品としては、例えば、エピクロン８６０、エピクロン１０５０、エピクロン１０５５、エピクロン２０５０、エピクロン３０５０、エピクロン４０５０、エピクロン７０５０、エピクロンＨＭ－０９１、エピクロンＨＭ－１０１、エピクロンＮ－７３０Ａ、エピクロンＮ－７４０、エピクロンＮ－７７０、エピクロンＮ－７７５、エピクロンＮ－８６５、エピクロンＨＰ－４０３２Ｄ、エピクロンＨＰ－７２００Ｌ、エピクロンＨＰ－７２００、エピクロンＨＰ－７２００Ｈ、エピクロンＨＰ－７２００ＨＨ、エピクロンＨＰ－７２００ＨＨＨ、エピクロンＨＰ－４７００、エピクロンＨＰ－４７１０、エピクロンＨＰ－４７７０、エピクロンＨＰ－５０００、エピクロンＨＰ－６０００、Ｎ５００Ｐ－２、及びＮ５００Ｐ－１０（以上、ＤＩＣ株式会社製の商品名）、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、ＥＯＣＮ－１０２Ｓ、ＥＯＣＮ－１０３Ｓ、ＥＯＣＮ－１０４Ｓ、ＣＥＲ－１０２０、ＥＰＰＮ－２０１、ＢＲＥＮ－Ｓ、ＢＲＥＮ－１０Ｓ（以上、日本化薬株式会社製の商品名）、ＹＸ－４０００、ＹＸ－４０００Ｈ、ＹＬ４１２１Ｈ、及びＹＸ－８８００（以上、三菱ケミカル株式会社製の商品名）、ＶＧ３１０１Ｌ（以上、株式会社プリンテック製の商品名）等が挙げられる。 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 is excellent in fluidity. The crystalline epoxy resin (highly crystalline epoxy resin) may contain, for example, at least one selected from the group consisting of a hydroquinone type epoxy resin, a bisphenol type epoxy resin, a thioether type epoxy resin, and a 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-865, Epicron HP-4032D, Epicron HP-7200L, Epicron HP-7200, Epicron HP-7200H, Epicron HP-7200HH, Epicron HP-7200HH, Epicron HP-4700, Epicron HP-4710, Epicron HP-4770, Epicron HP-5000, Epicron HP-6000, N500P-2, and N500P-10 (above, trade name manufactured by DIC Co., Ltd.), 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, HPEN-502H, EOCN-1020, EOCN-102S, EOCN-103S, EOCN-104S, CER-1020, EPPN-201, BREN-S, BREN-10S (above, trade name manufactured by Nippon Kayaku Co., Ltd.), YX -4000, YX-4000H, YL4121H, YX-8800 (above, trade name manufactured by Mitsubishi Chemical Co., Ltd.), VG3101L (above, trade name manufactured by Printec Co., Ltd.) and the like can be mentioned.
　樹脂組成物は、上記のうち一種のエポキシ樹脂を含有してよい。樹脂組成物は、上記のうち複数種のエポキシ樹脂を含有してもよい。樹脂組成物は、上記のエポキシ樹脂の中でも、ビフェニル骨格を含むエポキシ樹脂、オルソクレゾールノボラック型エポキシ樹脂、２個以上のエポキシ基を含む多官能型エポキシ樹脂を含有してよい。 The resin composition may contain one of the above epoxy resins. The resin composition may contain a plurality of types of epoxy resins among the above. Among the above epoxy resins, the resin composition may contain an epoxy resin containing a biphenyl skeleton, an orthocresol novolac type epoxy resin, and a polyfunctional epoxy resin containing two or more epoxy groups.
　硬化剤は、低温から室温の範囲でエポキシ樹脂を硬化させる硬化剤と、加熱に伴ってエポキシ樹脂を硬化させる加熱硬化型硬化剤と、に分類される。低温から室温の範囲でエポキシ樹脂を硬化させる硬化剤は、例えば、脂肪族ポリアミン、ポリアミノアミド、及びポリメルカプタン等である。加熱硬化型硬化剤は、例えば、芳香族ポリアミン、酸無水物、フェノールノボラック樹脂、及びジシアンジアミド（ＤＩＣＹ）等である。硬化剤の種類は特に制限されず、組成物の所望の特性等に応じて選択できる。 The curing agent is classified into a curing agent that cures the epoxy resin in the range of low temperature to room temperature and a heat curing type curing agent that cures the epoxy resin with heating. The curing agent that cures the epoxy resin in the range of low temperature to room temperature is, for example, aliphatic polyamines, polyaminoamides, and polymercaptans. The heat-curable curing agent is, for example, aromatic polyamine, acid anhydride, phenol novolac resin, dicyandiamide (DICY) and the like. The type of the curing agent is not particularly limited and can be selected according to the desired properties of the composition and the like.
　低温から室温の範囲でエポキシ樹脂を硬化させる硬化剤を用いた場合、エポキシ樹脂の硬化物のガラス転移点は低く、エポキシ樹脂の硬化物は軟らかい傾向がある。その結果、コンパウンドから形成された成型体も軟らかくなり易い。一方、成型体の耐熱性を向上させる観点から、硬化剤は、好ましくは加熱硬化型の硬化剤、より好ましくはフェノール樹脂、更に好ましくはフェノールノボラック樹脂であってよい。特に硬化剤としてフェノールノボラック樹脂を用いることで、ガラス転移点が高いエポキシ樹脂の硬化物が得られ易い。その結果、成型体の耐熱性及び機械的強度が向上し易い。 When a curing agent that cures the epoxy resin in the range from 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 body 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 phenol resin, and further preferably a phenol novolac resin. In particular, by using a phenol novolac resin as a curing agent, it is easy to obtain a cured product of an epoxy resin having a high glass transition point. As a result, the heat resistance and mechanical strength of the molded body are likely to be improved.
　フェノール樹脂は、例えば、アラルキル型フェノール樹脂、ジシクロペンタジエン型フェノール樹脂、サリチルアルデヒド型フェノール樹脂、ノボラック型フェノール樹脂、ベンズアルデヒド型フェノールとアラルキル型フェノールとの共重合型フェノール樹脂、パラキシリレン及び／又はメタキシリレン変性フェノール樹脂、メラミン変性フェノール樹脂、テルペン変性フェノール樹脂、ジシクロペンタジエン型ナフトール樹脂、シクロペンタジエン変性フェノール樹脂、多環芳香環変性フェノール樹脂、ビフェニル型フェノール樹脂、ビフェニレンアラルキル型フェノール樹脂、及びトリフェニルメタン型フェノール樹脂からなる群より選ばれる少なくとも一種を含んでいてよい。フェノール樹脂は、上記のうちの２種以上から構成される共重合体であってもよい。フェノール樹脂の市販品としては、例えば、荒川化学工業株式会社製のタマノル７５８、日立化成株式会社製のＨＰ－８５０Ｎ、明和化成株式会社製のＭＥＨＣ‐７５００－３Ｓ、ＭＥＨＣ‐７８５１ＳＳ等を用いてもよい。 The phenol resin is, for example, an aralkyl type phenol resin, a dicyclopentadiene type phenol resin, a salicylaldehyde type phenol resin, a novolak type phenol resin, a copolymerized phenol resin of a benzaldehyde type phenol and an aralkyl type phenol, a paraxylylene and / or a metaxylylene modification. Phenol resin, melamine-modified phenol resin, terpen-modified phenol resin, dicyclopentadiene-type naphthol resin, cyclopentadiene-modified phenol resin, polycyclic aromatic ring-modified phenol resin, biphenyl-type phenol resin, biphenylene aralkyl-type phenol resin, and triphenylmethane-type It may contain at least one selected from the group consisting of phenolic resins. The phenol resin may be a copolymer composed of two or more of the above. As commercially available phenolic resins, for example, Tamanol 758 manufactured by Arakawa Chemical Industry Co., Ltd., HP-850N manufactured by Hitachi Kasei Co., Ltd., MEHC-7500-3S manufactured by Meiwa Kasei Co., Ltd., MEHC-7851SS, etc. may be used. good.
　フェノールノボラック樹脂は、例えば、フェノール類及び／又はナフトール類と、アルデヒド類と、を酸性触媒下で縮合又は共縮合させて得られる樹脂であってよい。フェノールノボラック樹脂を構成するフェノール類は、例えば、フェノール、クレゾール、キシレノール、レゾルシン、カテコール、ビスフェノールＡ、ビスフェノールＦ、フェニルフェノール及びアミノフェノールからなる群より選ばれる少なくとも一種を含んでいてよい。フェノールノボラック樹脂を構成するナフトール類は、例えば、α－ナフトール、β－ナフトール及びジヒドロキシナフタレンからなる群より選ばれる少なくとも一種を含んでいてよい。フェノールノボラック樹脂を構成するアルデヒド類は、例えば、ホルムアルデヒド、アセトアルデヒド、プロピオンアルデヒド、ベンズアルデヒド及びサリチルアルデヒドからなる群より選ばれる少なくとも一種を含んでいてよい。 The phenol novolac resin may be, for example, a resin obtained by condensing or co-condensing phenols and / or naphthols and aldehydes under an acidic catalyst. The phenols constituting the phenol novolak resin may include, 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 novolak resin may contain, 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 contain, for example, at least one selected from the group consisting of formaldehyde, acetaldehyde, propionaldehyde, benzaldehyde and salicylaldehyde.
　硬化剤は、例えば、１分子中に２個のフェノール性水酸基を有する化合物であってもよい。１分子中に２個のフェノール性水酸基を有する化合物は、例えば、レゾルシン、カテコール、ビスフェノールＡ、ビスフェノールＦ、及び置換又は非置換のビフェノールからなる群より選ばれる少なくとも一種を含んでいてよい。 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 contain, for example, at least one selected from the group consisting of resorcin, catechol, bisphenol A, bisphenol F, and substituted or unsubstituted biphenol.
　樹脂組成物は、上記のうち一種のフェノール樹脂を含有してよい。樹脂組成物は、上記のうち複数種のフェノール樹脂を備えてもよい。樹脂組成物は、上記のうち一種の硬化剤を含有してよい。樹脂組成物は、上記のうち複数種の硬化剤を含有してもよい。 The resin composition may contain one of the above phenolic resins. The resin composition may include a plurality of types of phenol resins among the above. The resin composition may contain one of the above-mentioned curing agents. The resin composition may contain a plurality of types of curing agents among the above.
　エポキシ樹脂中のエポキシ基と反応する硬化剤中の活性基（フェノール性ＯＨ基）の比率は、エポキシ樹脂中のエポキシ基１当量に対して、好ましくは０．５～１．５当量、より好ましくは０．６～１．４当量、更に好ましくは０．７～１．２当量であってよい。硬化剤中の活性基の比率が０．５当量未満である場合、得られる硬化物の充分な弾性率が得られ難い。一方、硬化剤中の活性基の比率が１．５当量を超える場合、コンパウンドから形成された成型体の硬化後の機械的強度が低下する傾向がある。ただし、硬化剤中の活性基の比率が上記範囲外である場合であっても、本発明に係る効果は得られる。 The ratio of the active group (phenolic OH group) in the curing agent that reacts with the epoxy group in the epoxy resin is preferably 0.5 to 1.5 equivalents, more preferably 0.5 equivalents, relative to 1 equivalent of the epoxy group in the epoxy resin. May be 0.6 to 1.4 equivalents, more preferably 0.7 to 1.2 equivalents. When the ratio of active groups in the curing agent is less than 0.5 equivalent, it is difficult to obtain a sufficient elastic modulus of the obtained cured product. On the other hand, when 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 when the ratio of the active group in the curing agent is out of the above range, the effect according to the present invention can be obtained.
　樹脂組成物がリン酸エステルを含む分散剤を含有することで、コンパウンドの流動性を向上することができる。これにより、成型時の未充填、成型体中のボイド発生を抑制することができる。コンパウンドの流動性が向上する理由は必ずしも定かではないが、発明者らは、金属粉にリン酸エステルのリン酸基が選択的に吸着し、それにより金属粉の分散性が改善するため、流動性が向上するものと推察している。 By containing a dispersant containing a phosphoric acid ester in the resin composition, the fluidity of the compound can be improved. This makes it possible to suppress unfilling during molding and generation of voids in the molded body. The reason for the improved fluidity of the compound is not always clear, but the inventors have found that the phosphate groups of the phosphate ester are selectively adsorbed on the metal powder, which improves the dispersibility of the metal powder and thus flows. It is speculated that the sex will improve.
　リン酸エステルは、Ｏ＝Ｐ（ＯＨ）３－ｎ（ＯＲ）ｎ（ｎ＝１～３）で表される化合物である。リン酸エステルとしては、リン酸モノエステル、リン酸ジエステル又はリン酸トリエステルのいずれであってもよいが、コンパウンドの流動性を向上させる観点からは、上記式中のｎが１又は２である、リン酸モノエステル又はリン酸ジエステルであってよい。 The phosphoric acid ester is a compound represented by O = P (OH) 3-n (OR) n (n = 1 to 3). The phosphoric acid ester may be either a phosphoric acid monoester, a phosphoric acid diester or a phosphoric acid triester, but from the viewpoint of improving the fluidity of the compound, n in the above formula is 1 or 2. , Phosphoric acid monoester or phosphoric acid diester.
　リン酸エステルとしては、好ましくは－ＯＲ（Ｒは炭素数４以上の有機基を示す）で表される基を有してよい。エステル部位に含まれる有機基の炭素数が４以上であることによりコンパウンドの流動性を向上し易い。この観点から、Ｒの炭素数は５以上であってよく、６以上であってよい。また、金属粉の分散性の観点から、Ｒの炭素数は２０以下とすることができ、１５以下であってよい。 The phosphoric acid ester may preferably have a group represented by -OR (R indicates an organic group having 4 or more carbon atoms). When the number of carbon atoms of the organic group contained in the ester moiety is 4 or more, the fluidity of the compound can be easily improved. From this point of view, the carbon number of R may be 5 or more, and may be 6 or more. Further, from the viewpoint of dispersibility of the metal powder, the carbon number of R can be 20 or less, and may be 15 or less.
　有機基は、炭素数４以上のアルキル基、又は炭素数４以上のアルキル基中の炭素－炭素結合の少なくとも一部にエーテル結合が挿入された基であってよい。これにより、コンパウンドの流動性を向上し易い。アルキル基は、直鎖状又は分岐状アルキル基であってよい。 The organic group may be an alkyl group having 4 or more carbon atoms or a group in which an ether bond is inserted in at least a part of carbon-carbon bonds in an alkyl group having 4 or more carbon atoms. This makes it easy to improve the fluidity of the compound. The alkyl group may be a linear or branched alkyl group.
　アルキル基、及びアルキル基中の炭素－炭素結合の少なくとも一部にエーテル結合が挿入された基は、置換基（反応性基）を有していてよい。これにより、樹脂組成物に含まれる樹脂と分散剤との相溶性がより向上する。置換基としては、アミノ基、ウレイド基、エポキシ基、チオール基、（メタ）アクリロイル基、ヒドロキシ基等が挙げられる。なお、有機基Ｒにおける上記の「炭素数」は、置換基に含まれる炭素数を含まない数である。 The alkyl group and the group in which the ether bond is inserted in at least a part of the carbon-carbon bond in the alkyl group may have a substituent (reactive group). As a result, the compatibility between the resin contained in the resin composition and the dispersant is further improved. Examples of the substituent include an amino group, a ureido group, an epoxy group, a thiol group, a (meth) acryloyl group, a hydroxy group and the like. The above-mentioned "carbon number" in the organic group R is a number not including the carbon number contained in the substituent.
　リン酸エステルの市販品としては、例えば、城北化学工業株式会社製のＪＰ－５０４、ＪＰ－５０６Ｈ、ＪＰ－５０８、ＪＰ－５１３等が挙げられる。
　下記化学式１で表される化合物１は、例えば上記ＪＰ‐５０４であってよい。
　下記化学式２で表される化合物２は、例えば上記ＪＰ‐５０６Ｈであってよい。
　下記化学式３で表される化合物３は、例えば上記ＪＰ‐５０８であってよい。
　下記化学式４で表される化合物４は、例えば上記ＪＰ‐５１３であってよい。
（Ｃ４Ｈ９Ｏ）ｎＯＰ（ＯＨ）３－ｎ　（１）
　上記化学式１中のｎは、１又は２であってよい。上記化学式１中のｎは、１以上３以下であってもよい。
（Ｃ４Ｈ９ＯＣＨ２ＣＨ２Ｏ）ｎＯＰ（ＯＨ）３－ｎ　（２）
　上記化学式２中のｎは、１又は２であってよい。上記化学式２中のｎは、１以上３以下であってもよい。
（Ｃ４Ｈ９Ｃ２Ｈ５ＣＨＣＨ２Ｏ）ｎＯＰ（ＯＨ）３－ｎ　（３）
　上記化学式３中のｎは、１又は２であってよい。上記化学式３中のｎは、１以上３以下であってもよい。
（ｉｓо‐Ｃ１３Ｈ２７Ｏ）ｎＯＰ（ＯＨ）３－ｎ　（４）
　上記化学式４中のｎは、１又は２であってよい。上記化学式４中のｎは、１以上３以下であってもよい。 Examples of commercially available phosphoric acid esters include JP-504, JP-506H, JP-508, and JP-513 manufactured by Johoku Chemical Industry Co., Ltd.
The compound 1 represented by the following chemical formula 1 may be, for example, JP-504.
The compound 2 represented by the following chemical formula 2 may be, for example, JP-506H described above.
The compound 3 represented by the following chemical formula 3 may be, for example, JP-508.
The compound 4 represented by the following chemical formula 4 may be, for example, JP-513.
(C 4 H 9 O) n OP (OH) 3-n (1)
N in the above chemical formula 1 may be 1 or 2. N in the above chemical formula 1 may be 1 or more and 3 or less.
(C 4 H 9 OCH 2 CH 2 O) n OP (OH) 3-n (2)
N in the above chemical formula 2 may be 1 or 2. N in the above chemical formula 2 may be 1 or more and 3 or less.
(C 4 H 9 C 2 H 5 CHCH 2 O) n OP (OH) 3-n (3)
N in the above chemical formula 3 may be 1 or 2. N in the above chemical formula 3 may be 1 or more and 3 or less.
(Isо-C 13 H 27 O) n OP (OH) 3-n (4)
N in the above chemical formula 4 may be 1 or 2. N in the above chemical formula 4 may be 1 or more and 3 or less.
　分散剤の配合量は、コンパウンドの流動性を向上する観点から、１００質量部の金属粉に対して、１質量部以下、０．５質量部以下、０．１質量部以下、又は０．０５質量部以下であってよい。同様の観点から、当該配合量は０．０１質量部以上であってよい。 The blending amount of the dispersant is 1 part by mass or less, 0.5 part by mass or less, 0.1 part by mass or less, or 0.05 with respect to 100 parts by mass of the metal powder from the viewpoint of improving the fluidity of the compound. It may be less than or equal to a mass part. From the same viewpoint, the blending amount may be 0.01 parts by mass or more.
　硬化促進剤は、例えば、エポキシ樹脂と反応してエポキシ樹脂の硬化を促進させる組成物であれば限定されない。硬化促進剤は、例えば、リン系硬化促進剤、イミダゾール系硬化促進剤又はウレア系硬化促進剤であってよい。樹脂組成物が硬化促進剤を含有することで、コンパウンドの成型性及び離型性を向上することができる。また、樹脂組成物が硬化促進剤を含有することにより、コンパウンドを用いて製造された成型体又は硬化物（例えば、電子部品）の機械的強度が向上したり、高温・高湿な環境下におけるコンパウンドの保存安定性が向上したりする。 The curing accelerator is not limited as long as it is a composition that reacts with the epoxy resin to accelerate the curing of the epoxy resin, for example. The curing accelerator may be, for example, a phosphorus-based curing accelerator, an imidazole-based curing accelerator, or a urea-based curing accelerator. When the resin composition contains a curing accelerator, the moldability and releasability of the compound can be improved. Further, when the resin composition contains a curing accelerator, the mechanical strength of a molded product or a cured product (for example, an electronic component) manufactured by using a compound is improved, or in a high temperature and high humidity environment. The storage stability of the compound is improved.
　リン系硬化促進剤としては、例えば、ホスフィン化合物及びホスホニウム塩化合物が挙げられる。 Examples of the phosphorus-based curing accelerator include phosphine compounds and phosphonium salt compounds.
　イミダゾール系硬化促進剤の市販品としては、例えば、２ＭＺ‐Ｈ、Ｃ１１Ｚ、Ｃ１７Ｚ、１，２ＤＭＺ、２Ｅ４ＭＺ、２ＰＺ‐ＰＷ、２Ｐ４ＭＺ、１Ｂ２ＭＺ、１Ｂ２ＰＺ、２ＭＺ‐ＣＮ、Ｃ１１Ｚ‐ＣＮ、２Ｅ４ＭＺ‐ＣＮ、２ＰＺ‐ＣＮ、Ｃ１１Ｚ‐ＣＮＳ、２Ｐ４ＭＨＺ、ＴＰＺ、及びＳＦＺ（以上、四国化成工業株式会社製の商品名）からなる群より選ばれる少なくとも一種を用いてよい。 Commercially available imidazole-based curing accelerators include, for example, 2MZ-H, C11Z, C17Z, 1,2DMZ, 2E4MZ, 2PZ-PW, 2P4MZ, 1B2MZ, 1B2PZ, 2MZ-CN, C11Z-CN, 2E4MZ-CN, 2PZ. -At least one selected from the group consisting of CN, C11Z-CNS, 2P4MHZ, TPZ, and SFZ (above, trade name manufactured by Shikoku Chemicals Corporation) may be used.
　ウレア系硬化促進剤としては、ウレア基を有する硬化促進剤であれば特に限定されないが、保存安定性の向上の観点から、アルキルウレア基を有するアルキルウレア系硬化促進剤であることが好ましい。アルキルウレア基を有するアルキルウレア系硬化促進剤としては、芳香族アルキルウレア及び脂肪族アルキルウレアが挙げられる。アルキルウレア系硬化促進剤の市販品としては、例えば、Ｕ－ＣＡＴ３５１２Ｔ（商品名、サンアプロ株式会社製、芳香族ジメチルウレア）及びＵ－ＣＡＴ３５１３Ｎ（商品名、サンアプロ株式会社製、脂肪族ジメチルウレア）が挙げられる。これらの中でも、開裂温度が適度に低く、コンパウンドを効率的に硬化させ易いことから、芳香族アルキルウレアが好ましい。 The urea-based curing accelerator is not particularly limited as long as it is a curing accelerator having a urea group, but from the viewpoint of improving storage stability, an alkyl urea-based curing accelerator having an alkyl urea group is preferable. Examples of the alkylurea-based curing accelerator having an alkylurea group include aromatic alkylurea and aliphatic alkylurea. Examples of commercially available alkyl urea-based curing accelerators include U-CAT3512T (trade name, manufactured by San-Apro Co., Ltd., aromatic dimethyl urea) and U-CAT3513N (trade name, manufactured by San-Apro Co., Ltd., aliphatic dimethyl urea). Can be mentioned. Among these, aromatic alkylurea is preferable because the cleavage temperature is moderately low and the compound can be easily cured efficiently.
　硬化促進剤の配合量は、硬化促進効果が得られる量であればよく、特に限定されない。ただし、樹脂組成物の吸湿時の硬化性及び流動性を改善する観点からは、硬化促進剤の配合量は、１００質量部のエポキシ樹脂に対して、好ましくは０．１質量部以上３０質量部以下、より好ましくは１質量部以上１５質量部以下であってよい。硬化促進剤の含有量は、エポキシ樹脂及びフェノール樹脂の質量の合計１００質量部に対して０．００１質量部以上５質量部以下であることが好ましい。硬化促進剤の配合量が０．１質量部未満である場合、十分な硬化促進効果が得られ難い。硬化促進剤の配合量が３０質量部を超える場合、コンパウンドの保存安定性が低下し易い。ただし、硬化促進剤の配合量及び含有量が上記範囲外である場合であっても、本発明に係る効果は得られる。 The amount of the curing accelerator to be blended is not particularly limited as long as it can obtain the curing promoting effect. However, from the viewpoint of improving the curability and fluidity of the resin composition during moisture absorption, the amount of the curing accelerator is preferably 0.1 part by mass or more and 30 parts by mass with respect to 100 parts by mass of the epoxy resin. Hereinafter, it may be more preferably 1 part by mass or more and 15 parts by mass or less. The content of the curing accelerator is preferably 0.001 part by mass or more and 5 parts by mass or less with respect to 100 parts by mass of the total mass of the epoxy resin and the phenol resin. When the blending amount of the curing accelerator is less than 0.1 parts by mass, it is difficult to obtain a sufficient curing promoting effect. When the blending amount of the curing accelerator exceeds 30 parts by mass, the storage stability of the compound tends to decrease. However, even when the blending amount and content of the curing accelerator are out of the above range, the effect according to the present invention can be obtained.
　カップリング剤は、樹脂組成物と、金属粉を構成する金属元素含有粒子との密着性を向上させ、コンパウンドから形成される成型体の可撓性及び機械的強度を向上させる。カップリング剤は、例えば、シラン系化合物（シランカップリング剤）、チタン系化合物、アルミニウム化合物（アルミニウムキレート類）、及びアルミニウム／ジルコニウム系化合物からなる群より選ばれる少なくとも一種であってよい。シランカップリング剤は、例えば、エポキシシラン、メルカプトシラン、アミノシラン、アルキルシラン、ウレイドシラン、酸無水物系シラン、ビニルシラン及び（メタ）アクリロイルオキシシランからなる群より選ばれる少なくとも一種であってよい。樹脂組成物は、上記のうち一種のカップリング剤を含有してよく、上記のうち複数種のカップリング剤を含有してもよい。 The coupling agent improves the adhesion between the resin composition and the metal element-containing particles constituting the metal powder, and improves the flexibility and mechanical strength of the molded product formed from the compound. The coupling agent may be, for example, at least one selected from the group consisting of a silane compound (silane coupling agent), a titanium compound, an aluminum compound (aluminum chelate), and an aluminum / zirconium compound. The silane coupling agent may be at least one selected from the group consisting of, for example, epoxysilane, mercaptosilane, aminosilane, alkylsilane, ureidosilane, acid anhydride-based silane, vinylsilane and (meth) acryloyloxysilane. The resin composition may contain one of the above-mentioned coupling agents, and may contain a plurality of of the above-mentioned coupling agents.
　コンパウンドの成型収縮率が低減され易く、また成型体の耐熱性及び耐電圧性が向上し易いことから、樹脂組成物は、シロキサン結合を有する化合物（シロキサン化合物）を含有してもよい。シロキサン結合は、２つのケイ素原子（Ｓｉ）と１つの酸素原子（Ｏ）とを含む結合であり、－Ｓｉ－Ｏ－Ｓｉ－で表されてよい。シロキサン結合を有する化合物はポリシロキサン化合物であってよい。 The resin composition may contain a compound having a siloxane bond (siloxane compound) because the molding shrinkage rate of the compound is easily reduced and the heat resistance and withstand voltage resistance of the molded product are easily improved. 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.
　コンパウンドの環境安全性、リサイクル性、成型加工性及び低コストのために、コンパウンドは難燃剤を含んでよい。難燃剤は、例えば、臭素系難燃剤、リン系難燃剤、水和金属化合物系難燃剤、シリコーン系難燃剤、窒素含有化合物、ヒンダードアミン化合物、有機金属化合物及び芳香族エンプラからなる群より選ばれる少なくとも一種であってよい。樹脂組成物は、上記のうち一種の難燃剤を含有してよく、上記のうち複数種の難燃剤を含有してもよい。 The compound may contain flame retardants due to the environmental safety, recyclability, moldability and low cost of the compound. The flame retardant is at least selected from the group consisting of, for example, a bromine-based flame retardant, a phosphorus-based flame retardant, a hydrated metal compound-based flame retardant, a silicone-based flame retardant, a nitrogen-containing compound, a hindered amine compound, an organic metal compound, and an aromatic empra. It may be a kind. The resin composition may contain one of the above flame retardants, and may contain a plurality of of the above flame retardants.
　金型を用いてコンパウンドから成型体を形成する場合、樹脂組成物は、離型剤を含有してよい。離型剤は、コンパウンドの成型（例えばトランスファー成型）におけるコンパウンドの流動性を向上する剤としても機能する。離型剤としては、高級脂肪酸等の脂肪酸、脂肪酸エステル、脂肪酸金属塩などが挙げられる。 When forming a molded body from a compound using a mold, the resin composition may contain a mold release agent. The mold release agent also functions as an agent for improving the fluidity of the compound in the molding of the compound (for example, transfer molding). Examples of the release agent include fatty acids such as higher fatty acids, fatty acid esters, and fatty acid metal salts.
　離型剤は、例えば、モンタン酸、ステアリン酸、１２－オキシステアリン酸、ラウリン酸等の脂肪酸類又はこれらのエステル（例えばアルキルエステル）；ステアリン酸亜鉛、ステアリン酸カルシウム、ステアエン酸バリウム、ステアリン酸アルミニウム、ステアリン酸マグネシウム、ラウリン酸カルシウム、リノール酸亜鉛、リシノール酸カルシウム、２－エチルヘキソイン酸亜鉛等の脂肪酸塩；ステアリン酸アミド、オレイン酸アミド、エルカ酸アミド、ベヘン酸アミド、パルミチン酸アミド、ラウリン酸アミド、ヒドロキシステアリン酸アミド、メチレンビスステアリン酸アミド、エチレンビスステアリン酸アミド、エチレンビスラウリン酸アミド、ジステアリルアジピン酸アミド、エチレンビスオレイン酸アミド、ジオレイルアジピン酸アミド、Ｎ－ステアリルステアリン酸アミド、Ｎ－オレイルステアリン酸アミド、Ｎ－ステアリルエルカ酸アミド、メチロールステアリン酸アミド、メチロールベヘン酸アミド等の脂肪酸アミド；エチレングリコール、ステアリルアルコール等のアルコール類；ポリエチレングリコール、ポリプロピレングリコール、ポリテトラメチレングリコール及びこれらの変性物からなるポリエーテル類；フッ素系オイル、フッ素系グリース、含フッ素樹脂粉末等のフッ素化合物；並びに、パラフィンワックス、ポリエチレンワックス、アマイドワックス、ポリプロピレンワックス、エステルワックス、カルナウバ、マイクロワックス等のワックス類；からなる群より選ばれる少なくとも一種であってよい。 The release agent is, for example, fatty acids such as montanic acid, stearic acid, 12-oxystearic acid, lauric acid or esters thereof (for example, alkyl esters); zinc stearate, calcium stearate, barium steaenoate, aluminum stearate, etc. Fatty acid salts such as magnesium stearate, calcium laurate, zinc linoleate, calcium lysinolate, zinc 2-ethylhexoneate; stearic acid amide, oleate amide, erucic acid amide, behenic acid amide, palmitate amide, lauric acid amide, hydroxy Stearic acid amide, methylene bisstearic acid amide, ethylene bisstearic acid amide, ethylene bislauric acid amide, distealyl adipic acid amide, ethylene bisoleic acid amide, diorail adipic acid amide, N-stearyl stearic acid amide, N-oleyl Stearic acid amides, N-stearyl erucate amides, methylol stearic acid amides, methylol behenic acid amides and other fatty acid amides; alcohols such as ethylene glycol and stearyl alcohol; polyethylene glycols, polypropylene glycols, polytetramethylene glycols and modified products thereof. Polyethers consisting of; fluorine compounds such as fluorine oil, fluorine grease, and fluorine-containing resin powder; and waxes such as paraffin wax, polyethylene wax, amido wax, polypropylene wax, ester wax, carnauba, and microwax; It may be at least one selected from the group of
（金属粉）
　金属粉（金属元素含有粒子）は、例えば、金属単体、合金及び金属化合物からなる群より選ばれる少なくとも一種を含有してよい。金属粉は、例えば、金属単体、合金及び金属化合物からなる群より選ばれる少なくとも一種からなっていてよい。合金は、固溶体、共晶及び金属間化合物からなる群より選ばれる少なくとも一種を含んでよい。合金とは、例えば、ステンレス鋼（Ｆｅ‐Ｃｒ系合金、Ｆｅ‐Ｎｉ‐Ｃｒ系合金等）であってよい。金属化合物とは、例えば、フェライト等の酸化物であってよい。金属粉は、一種の金属元素又は複数種の金属元素を含んでよい。金属粉に含まれる金属元素は、例えば、卑金属元素、貴金属元素、遷移金属元素、又は希土類元素であってよい。コンパウンドは、一種の金属粉を含んでよく、組成が異なる複数種の金属粉を含んでもよい。 (Metal powder)
The metal powder (particle containing a metal element) may contain, for example, at least one selected from the group consisting of elemental metals, alloys and metal compounds. The metal powder may consist of, for example, at least one selected from the group consisting of elemental metals, alloys and metal compounds. The alloy may contain at least one selected from the group consisting of solid solutions, eutectic and intermetallic compounds. The alloy may be, for example, stainless steel (Fe—Cr based alloy, Fe—Ni—Cr based alloy, etc.). The metal compound may be, for example, an oxide such as ferrite. The metal powder may contain one kind of metal element or a plurality of kinds of metal elements. The metal element contained in the metal powder may be, for example, a base metal element, a noble metal element, a transition metal element, or a rare earth element. The compound may contain one kind of metal powder, and may contain a plurality of kinds of metal powder having different compositions.
　金属粉は上記の組成物に限定されない。金属粉に含まれる金属元素は、例えば、鉄（Ｆｅ）、銅（Ｃｕ）、チタン（Ｔｉ）、マンガン（Ｍｎ）、コバルト（Ｃｏ）、ニッケル（Ｎｉ）、亜鉛（Ｚｎ）、アルミニウム（Ａｌ）、スズ（Ｓｎ）、クロム（Ｃｒ）、ニオブ（Ｎｂ）、バリウム（Ｂａ）、ストロンチウム（Ｓｒ）、鉛（Ｐｂ）、銀（Ａｇ）、プラセオジム（Ｐｒ）、ネオジム（Ｎｄ）、サマリウム（Ｓｍ）及びジスプロシウム（Ｄｙ）からなる群より選ばれる少なくとも一種であってよい。金属粉は、金属元素以外の元素を更に含んでもよい。金属粉は、例えば、炭素（Ｃ）、酸素（О）、ベリリウム（Ｂｅ）、リン（Ｐ）、硫黄（Ｓ）、ホウ素（Ｂ）、又はケイ素（Ｓｉ）を含んでもよい。 The metal powder is not limited to the above composition. The metal elements contained in the metal powder are, for example, iron (Fe), copper (Cu), titanium (Ti), manganese (Mn), cobalt (Co), nickel (Ni), zinc (Zn), and aluminum (Al). , Tin (Sn), Chromium (Cr), Niob (Nb), Barium (Ba), Strontium (Sr), Lead (Pb), Silver (Ag), Placeodim (Pr), Neodim (Nd), Samalium (Sm) And at least one selected from the group consisting of dysprosium (Dy). The metal powder may further contain an element other than the metal element. The metal powder may contain, for example, carbon (C), oxygen (О), beryllium (Be), phosphorus (P), sulfur (S), boron (B), or silicon (Si).
　金属粉は、磁性粉であってよい。金属粉は、軟磁性合金、又は強磁性合金であってよい。金属粉は、例えば、Ｆｅ‐Ｓｉ系合金、Ｆｅ‐Ｓｉ‐Ａｌ系合金（センダスト）、Ｆｅ‐Ｎｉ系合金（パーマロイ）、Ｆｅ‐Ｃｕ‐Ｎｉ系合金（パーマロイ）、Ｆｅ‐Ｃｏ系合金（パーメンジュール）、Ｆｅ‐Ｃｒ‐Ｓｉ系合金（電磁ステンレス鋼）、Ｎｄ‐Ｆｅ‐Ｂ系合金（希土類磁石）、Ｓｍ‐Ｆｅ‐Ｎ系合金（希土類磁石）、Ａｌ‐Ｎｉ‐Ｃｏ系合金（アルニコ磁石）及びフェライトからなる群より選ばれる少なくとも一種からなる磁性粉であってよい。フェライトは、例えば、スピネルフェライト、六方晶フェライト、又はガーネットフェライトであってよい。金属粉は、Ｃｕ‐Ｓｎ系合金、Ｃｕ‐Ｓｎ‐Ｐ系合金、Ｃｕ‐Ｎｉ系合金、又はＣｕ‐Ｂｅ系合金等の銅合金であってもよい。金属粉は、上記の元素及び組成物のうち一種を含んでよく、上記の元素及び組成物のうち複数種を含んでもよい。 The metal powder may be a magnetic powder. The metal powder may be a soft magnetic alloy or a ferromagnetic alloy. The metal powder is, for example, Fe-Si alloy, Fe—Si—Al alloy (Sendust), Fe—Ni alloy (Permalloy), Fe—Cu—Ni alloy (Permalloy), Fe—Co alloy (Permalloy). Menzur), 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 (Arnico) It may be a magnetic powder consisting of at least one selected from the group consisting of (magnet) and ferrite. The ferrite may be, for example, spinel ferrite, hexagonal ferrite, or garnet ferrite. The metal powder may be a copper alloy such as a Cu—Sn based alloy, a Cu—Sn—P based alloy, a Cu—Ni based alloy, or a Cu—Be based alloy. The metal powder may contain one of the above elements and compositions, and may contain a plurality of of the above elements and compositions.
　金属粉は、Ｆｅ単体であってもよい。金属粉は、鉄を含む合金（Ｆｅ系合金）であってもよい。Ｆｅ系合金は、例えば、Ｆｅ‐Ｓｉ‐Ｃｒ系合金、又はＮｄ‐Ｆｅ‐Ｂ系合金であってよい。金属粉は、アモルファス系鉄粉及びカルボニル鉄粉のうちの少なくともいずれかであってもよい。金属粉がＦｅ単体及びＦｅ系合金のうちの少なくともいずれかを含む場合、高い占積率を有し、且つ磁気特性に優れる成型体をコンパウンドから作製し易い。金属粉は、Ｆｅアモルファス合金であってもよい。 The metal powder may be Fe alone. The metal powder may be an alloy containing iron (Fe-based alloy). The Fe-based alloy may be, for example, a Fe—Si—Cr based alloy or an Nd—Fe—B based alloy. The metal powder may be at least one of amorphous iron powder and carbonyl iron powder. When the metal powder contains at least one of Fe simple substance and Fe-based alloy, it is easy to produce a molded product having a high space factor and excellent magnetic properties from the compound. The metal powder may be an Fe amorphous alloy.
　Ｆｅアモルファス合金粉の市販品としては、例えば、ＡＷ２‐０８、ＫＵＡＭＥＴ‐６Ｂ２、９Ａ４－ＩＩ（以上、エプソンアトミックス株式会社製の商品名）、ＤＡＰ　ＭＳ３、ＤＡＰ　ＭＳ７、ＤＡＰ　ＭＳＡ１０、ＤＡＰ　ＰＢ、ＤＡＰ　ＰＣ、ＤＡＰ　ＭＫＶ４９、ＤＡＰ　４１０Ｌ、ＤＡＰ　４３０Ｌ、ＤＡＰ　ＨＹＢシリーズ（以上、大同特殊鋼株式会社製の商品名）、ＭＨ４５Ｄ、ＭＨ２８Ｄ、ＭＨ２５Ｄ、及びＭＨ２０Ｄ（以上、神戸製鋼株式会社製の商品名）からなる群より選ばれる少なくとも一種が用いられてよい。 Commercially available Fe amorphous alloy powders include, for example, AW2-08, KUAMET-6B2, 9A4-II (above, trade name manufactured by Epson Atmix Co., Ltd.), DAP MS3, DAP MS7, DAP MSA10, DAP PB, DAP. Consists of PC, DAP MKV49, DAP 410L, DAP 430L, DAP HYB series (above, product name manufactured by Daido Special Steel Co., Ltd.), MH45D, MH28D, MH25D, and MH20D (above, product name manufactured by Kobe Steel Co., Ltd.). At least one selected from the group may be used.
　コンパウンドは、金属粉と樹脂組成物（樹脂組成物を構成する各成分）とを加熱しながら混合することで製造される。例えば、金属粉と樹脂組成物とを加熱しながらニーダー、ロール、攪拌機などで混練してよい。金属粉及び樹脂組成物の加熱及び混合により、樹脂組成物が金属粉を構成する金属元素含有粒子の表面の一部又は全体に付着して金属元素含有粒子を被覆し、樹脂組成物中のエポキシ樹脂の一部又は全部が半硬化物になる。その結果、コンパウンドが得られる。金属粉及び樹脂組成物の加熱及び混合によって得られた粉末に、更にワックスを加えることによって、コンパウンドを得てもよい。予め樹脂組成物とワックスとが混合されていてもよい。 The compound is produced by mixing the metal powder and the resin composition (each component constituting the resin composition) while heating. For example, the metal powder and the resin composition may be kneaded with a kneader, a roll, a stirrer, or the like while heating. By heating and mixing the metal 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 powder to cover the metal element-containing particles, and the epoxy in the resin composition. Part or all of the resin becomes a semi-cured product. The result is a compound. A compound may be obtained by further adding wax to the powder obtained by heating and mixing the metal powder and the resin composition. The resin composition and the wax may be mixed in advance.
　混練では、金属粉、エポキシ樹脂、硬化剤、分散剤、硬化促進剤及びカップリング剤を槽内で混練してよい。金属粉、分散剤及びカップリング剤を槽内に投入して混合した後、エポキシ樹脂、硬化剤、及び硬化促進剤を槽内へ投入して、槽内の原料を混練してもよい。金属粉、分散剤、エポキシ樹脂、硬化剤及びカップリング剤を槽内で混練した後、硬化促進剤を槽内入れて、更に槽内の原料を混練してもよい。予めエポキシ樹脂、硬化剤、硬化促進剤及び分散剤の混合物（樹脂混合物）を作製して、続いて、金属粉及びカップリング剤を混練して金属混合物を作製して、続いて、金属混合物と上記の樹脂混合物とを混練してもよい。離型剤を用いる場合は、分散剤と同様のタイミングで配合するとよい。シロキサン化合物を用いる場合は、カップリング剤と同様のタイミングで配合するとよい。 In kneading, metal powder, epoxy resin, curing agent, dispersant, curing accelerator and coupling agent may be kneaded in the tank. After the metal powder, the dispersant 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 and the raw materials in the tank may be kneaded. After kneading the metal powder, the dispersant, the epoxy resin, the curing agent and the coupling agent in the tank, the curing accelerator may be put in the tank and the raw materials in the tank may be further kneaded. A mixture (resin mixture) of an epoxy resin, a curing agent, a curing accelerator and a dispersant is prepared in advance, and then a metal powder and a coupling agent are kneaded to prepare a metal mixture, and then a metal mixture is prepared. You may knead with the above resin mixture. When a mold release agent is used, it may be blended at the same timing as the dispersant. When a siloxane compound is used, it may be blended at the same timing as the coupling agent.
　混練時間は、混練機械の種類、混練機械の容積、コンパウンドの製造量にもよるが、例えば、１分以上であることが好ましく、２分以上であることがより好ましく、３分以上であることが更に好ましい。また、混練時間は、２０分以下であることが好ましく、１５分以下であることがより好ましく、１０分以下であることが更に好ましい。混練時間が１分未満である場合、混練が不十分であり、コンパウンドの成型性が損なわれ、コンパウンドの硬化度にばらつきが生じ易い。混練時間が２０分を超える場合、例えば、槽内で樹脂組成物（例えばエポキシ樹脂及び硬化剤）の硬化が進み、コンパウンドの流動性及び成型性が損なわれ易い。槽内の原料を加熱しながらニーダーで混練する場合、加熱温度は、例えば、エポキシ樹脂の半硬化物（Ｂステージのエポキシ樹脂）が生成し、且つエポキシ樹脂の硬化物（Ｃステージのエポキシ樹脂）の生成が抑制される温度であればよい。加熱温度は、硬化促進剤の活性化温度よりも低い温度であってよい。加熱温度は、例えば、５０℃以上であることが好ましく、６０℃以上であることがより好ましく、７０℃以上であることが更に好ましい。加熱温度は、１５０℃以下であることが好ましく、１２０℃以下であることがより好ましく、１１０℃以下であることが更に好ましい。加熱温度が上記の範囲内である場合、槽内の樹脂組成物が軟化して金属粉を構成する金属元素含有粒子の表面を被覆し易く、エポキシ樹脂の半硬化物が生成し易く、混練中のエポキシ樹脂の完全な硬化が抑制され易い。 The kneading time depends on the type of the kneading machine, the volume of the kneading machine, and the production amount of the compound, but for example, it is preferably 1 minute or more, more preferably 2 minutes or more, and 3 minutes or more. Is more preferable. The kneading time is preferably 20 minutes or less, more preferably 15 minutes or less, and even more preferably 10 minutes or less. When the kneading time is less than 1 minute, the kneading is insufficient, the moldability of the compound is impaired, and the degree of curing of the compound tends to vary. When the kneading time exceeds 20 minutes, for example, the resin composition (for example, epoxy resin and curing agent) is cured in the tank, and the fluidity and moldability of the compound are easily impaired. When the raw materials in the tank are kneaded with a kneader while heating, the heating temperature is, for example, a semi-cured epoxy resin (B-stage epoxy resin) and a cured epoxy resin (C-stage epoxy resin). It suffices as long as it is a temperature at which the formation of the epoxy is suppressed. The heating temperature may be 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 easily covers the surface of the metal element-containing particles constituting the metal powder, and a semi-cured epoxy resin is easily produced, and is being kneaded. Complete curing of the epoxy resin is likely to be suppressed.
［成型体及び硬化物］
　本実施形態に係る成型体は、上記のコンパウンドを備えてよい。本実施形態に係る硬化物は、上記のコンパウンドを硬化してなるものであり、上記の成型体に含まれていてよい。成型体は、未硬化の樹脂組成物、樹脂組成物の半硬化物（Ｂステージの樹脂組成物）、及び樹脂組成物の硬化物（Ｃステージの樹脂組成物）からなる群より選ばれる少なくとも一種を含んでいてよい。本実施形態に係る成型体は、電子部品又は電子回路基板用の封止材として用いられてよい。それにより、電子部品又は電子回路基板が備える金属部材と、成型体（封止材）との熱膨張率差に起因する成型体のクラックを抑制することができる。 [Molded body and cured product]
The molded body according to the present embodiment may be provided with the above-mentioned compound. The cured product according to the present embodiment is obtained by curing the above-mentioned compound, and may be contained in the above-mentioned molded body. The molded body is at least one selected from the group consisting of an uncured resin composition, a semi-cured resin composition (B-stage resin composition), and a cured resin composition (C-stage resin composition). May include. The molded body according to the present embodiment may be used as a sealing material for an electronic component or an electronic circuit board. Thereby, it is possible to suppress cracks in the molded body due to the difference in the coefficient of thermal expansion between the metal member included in the electronic component or the electronic circuit board and the molded body (sealing material).
　成型体は、コンパウンドを金型中で加圧する工程を備える製造方法により製造される。成型体の製造方法は、金属部材の表面の一部又は全体を覆うコンパウンドを金型中で加圧する工程を備えてよい。成型体の製造方法は、コンパウンドを金型中で加圧する工程のみを備えてよく、当該工程に加えてその他の工程を備えてもよい。成型体の製造方法は、第一工程、第二工程及び第三工程を備えてもよい。以下では、各工程の詳細を説明する。 The molded body is manufactured by a manufacturing method including a step of pressurizing the compound in a mold. The method for producing a molded body may include a step of pressurizing a compound covering a part or the whole of the surface of a metal member in a mold. The method for producing the molded body may include only the step of pressurizing the compound in the mold, and may include other steps in addition to the step. The method for producing the molded body may include a first step, a second step, and a third step. Hereinafter, the details of each step will be described.
　第一工程では、上記の方法でコンパウンドを作製する。 In the first step, the compound is prepared by the above method.
　第二工程では、コンパウンドを金型中で加圧することにより、成型体（Ｂステージの成型体）を得る。第二工程では、金属部材の表面の一部又は全体を覆うコンパウンドを金型中で加圧することにより、成型体（Ｂステージの成型体）を得てよい。第二工程において、樹脂組成物が、金属粉を構成する個々の金属元素含有粒子間に充填される。そして樹脂組成物は、結合材（バインダ）として機能し、金属元素含有粒子同士を互いに結着する。 In the second step, a molded body (B stage molded body) is obtained by pressurizing the compound in the mold. In the second step, a molded body (B stage molded body) may be obtained by pressing a compound covering a part or the whole of the surface of the metal member in the mold. In the second step, the resin composition is filled between the individual metal element-containing particles constituting the metal powder. The resin composition then functions as a binder and binds the metal element-containing particles to each other.
　第二工程として、コンパウンドのトランスファー成型を実施してもよい。トランスファー成型では、コンパウンドを３ＭＰａ以上５０ＭＰａ以下で加圧してよい。成型圧力が高いほど、機械的強度に優れた成型体が得られ易い傾向がある。成型体の量産性及び金型の寿命を考慮した場合、成型圧力は８ＭＰａ以上２０ＭＰａ以下であることが好ましい。トランスファー成型によって形成される成型体の密度は、コンパウンドの真密度に対して、好ましくは７５％以上８６％以下、より好ましくは８０％以上８６％以下であってよい。成型体の密度が７５％以上８６％以下である場合、機械的強度に優れた成型体が得られ易い。トランスファー成型において、第二工程と第三工程とを一括して実施してもよい。 As the second step, transfer molding of the compound may be carried out. In transfer molding, the compound may be pressurized at 3 MPa or more and 50 MPa or less. The higher the molding pressure, the easier it is to obtain a molded body having excellent mechanical strength. Considering 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 product formed by transfer molding may be preferably 75% or more and 86% or less, and more preferably 80% or more and 86% or less with respect to the true density of the compound. When the density of the molded body is 75% or more and 86% or less, it is easy to obtain a molded body having excellent mechanical strength. In the transfer molding, the second step and the third step may be carried out collectively.
　第三工程では、成型体を熱処理によって硬化させ、Ｃステージの成型体を得る。熱処理の温度は、成型体中の樹脂組成物が十分に硬化する温度であればよい。熱処理の温度は、好ましくは１００℃以上３００℃以下、より好ましくは１１０℃以上２５０℃以下であってよい。成型体中の金属粉の酸化を抑制するために、熱処理を不活性雰囲気下で行うことが好ましい。熱処理温度が３００℃を超える場合、熱処理の雰囲気に不可避的に含まれる微量の酸素によって金属粉が酸化されたり、樹脂硬化物が劣化したりする。金属粉の酸化、及び樹脂硬化物の劣化を抑制しながら樹脂組成物を十分に硬化させるためには、熱処理温度の保持時間は、好ましくは数分以上１０時間以下、より好ましくは３分以上８時間以下であってよい。 In the third step, the molded body is cured by heat treatment to obtain a C-stage molded body. The temperature of the heat treatment may be any temperature as long as the resin composition in the molded body is sufficiently cured. The temperature of the heat treatment may be preferably 100 ° C. or higher and 300 ° C. or lower, and more preferably 110 ° C. or higher and 250 ° C. or lower. In order to suppress the oxidation of the metal powder in the molded body, it is preferable to carry out the heat treatment in an inert atmosphere. When the heat treatment temperature exceeds 300 ° C., the metal powder is oxidized or the cured resin product is deteriorated by 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 powder and the deterioration of the cured resin product, the heat treatment temperature holding time is preferably several minutes or more and 10 hours or less, more preferably 3 minutes or more 8 It may be less than an hour.
　以下では実施例及び比較例により本発明を更に詳細に説明するが、本発明はこれらの例によって何ら限定されるものではない。 Hereinafter, the present invention will be described in more detail with reference to Examples and Comparative Examples, but the present invention is not limited to these examples.
　実施例及び比較例のコンパウンドの調製に使用した各成分の詳細を以下に示す。 Details of each component used in the preparation of the compounds of Examples and Comparative Examples are shown below.
（エポキシ樹脂）
・ビフェニレンアラルキル型エポキシ樹脂（日本化薬株式会社製の商品名：ＮＣ‐３０００、エポキシ当量：２７５ｇ／ｅｑ）
・３官能型エポキシ樹脂（株式会社プリンテック製の商品名：ＶＧ３１０１Ｌ、エポキシ当量：２１２ｇ／ｅｑ） (Epoxy resin)
-Biphenylene aralkyl type epoxy resin (trade name: NC-3000, epoxy equivalent: 275 g / eq manufactured by Nippon Kayaku Co., Ltd.)
-Trifunctional epoxy resin (trade name: VG3101L manufactured by Printec Co., Ltd., epoxy equivalent: 212 g / eq)
（硬化剤）
・トリフェニルメタン型フェノール樹脂（明和化成株式会社製の商品名：ＭＥＨＣ‐７５００－３Ｓ、水酸基当量：１０３ｇ／ｅｑ）
・ビフェニレンアラルキル型フェノール樹脂（明和化成株式会社製の商品名：ＭＥＨＣ‐７８５１ＳＳ、水酸基当量：２０２ｇ／ｅｑ） (Hardener)
-Triphenylmethane type phenol resin (trade name: MEHC-7500-3S manufactured by Meiwa Kasei Co., Ltd., hydroxyl group equivalent: 103 g / eq)
Biphenylene aralkyl type phenol resin (trade name: MEHC-7851SS manufactured by Meiwa Kasei Co., Ltd., hydroxyl group equivalent: 202 g / eq)
（硬化促進剤）
・イミダゾール系硬化促進剤（四国化成工業株式会社製の商品名：２Ｅ４ＭＺ） (Hardening accelerator)
-Imidazole-based curing accelerator (trade name: 2E4MZ manufactured by Shikoku Chemicals Corporation)
（カップリング剤）
・メタクリロキシオクチルトリメトキシシラン（信越化学工業株式会社製の商品名：ＫＢＭ－５８０３）
・３－グリシドキシプロピルトリエトキシシラン（信越化学工業株式会社製の商品名：ＫＢＭ－４０３） (Coupling agent)
・ Methaloxyoctyltrimethoxysilane (trade name: KBM-5803 manufactured by Shin-Etsu Chemical Co., Ltd.)
-3-glycidoxypropyltriethoxysilane (trade name: KBM-403 manufactured by Shin-Etsu Chemical Co., Ltd.)
（シロキサン化合物）
・カプロラクトン変性ジメチルシリコーン（Ｇｅｌｅｓｔ株式会社製の商品名：ＤＢＬ‐Ｃ３２） (Siloxane compound)
-Caprolactone-modified dimethyl silicone (trade name: DBL-C32 manufactured by Gelest Co., Ltd.)
（分散剤）
「－ＯＲ」で表される基を有する以下のリン酸エステル
・Ｒが炭素数４の有機基であるリン酸エステル（城北化学工業株式会社製の商品名：ＪＰ－５０４）
・Ｒが炭素数６の有機基であるリン酸エステル（城北化学工業株式会社製の商品名：ＪＰ－５０６Ｈ）
・Ｒが炭素数８の有機基であるリン酸エステル（城北化学工業株式会社製の商品名：ＪＰ－５０８）
・Ｒが炭素数１３の有機基であるリン酸エステル（城北化学工業株式会社製の商品名：ＪＰ－５１３） (Dispersant)
The following phosphoric acid ester having a group represented by "-OR" · R is an organic group having 4 carbon atoms (trade name: JP-504 manufactured by Johoku Chemical Industry Co., Ltd.)
-Phosphoric acid ester in which R is an organic group having 6 carbon atoms (trade name: JP-506H manufactured by Johoku Chemical Industry Co., Ltd.)
-Phosphoric acid ester in which R is an organic group having 8 carbon atoms (trade name: JP-508 manufactured by Johoku Chemical Industry Co., Ltd.)
-Phosphoric acid ester in which R is an organic group having 13 carbon atoms (trade name: JP-513 manufactured by Johoku Chemical Industry Co., Ltd.)
（離型剤）
・部分ケン化モンタン酸エステルワックス（クラリアントケミカルズ株式会社製の商品名：ＬＩＣＯＷＡＸ‐ＯＰ）
・ステアリン酸亜鉛（日油株式会社製の商品名：ジンクステアレート） (Release agent)
-Partially saponified montanic acid ester wax (trade name: LICOWAX-OP manufactured by Clariant Chemicals Co., Ltd.)
・ Zinc stearate (trade name: Zinc stearate manufactured by NOF CORPORATION)
（金属粉）
・アモルファス系鉄粉（エプソンアトミックス株式会社製の商品名：９Ａ４－ＩＩ、平均粒径２４μｍ）
・アモルファス系鉄粉（エプソンアトミックス株式会社製の商品名：ＡＷ２‐０８、平均粒径５．３μｍ） (Metal powder)
Amorphous iron powder (trade name: 9A4-II manufactured by Epson Atmix Co., Ltd., average particle size 24 μm)
Amorphous iron powder (trade name: AW2-08, average particle size 5.3 μm manufactured by Epson Atmix Co., Ltd.)
［コンパウンドの調製］
（実施例）
　表１に示すエポキシ樹脂、硬化剤、硬化促進剤、分散剤及び離型剤を、同表に示す配合量（単位：ｇ）でポリ容器に投入した。これらの材料をポリ容器内で１０分間混合することにより、樹脂混合物を調製した。樹脂混合物とは、樹脂組成物のうちカップリング剤及びシロキサン化合物を除く他の全成分に相当する。 [Preparation of compound]
(Example)
The epoxy resin, curing agent, curing accelerator, dispersant and mold release agent shown in Table 1 were put into a plastic container in the blending amounts (unit: g) shown in the same table. A resin mixture was prepared by mixing these materials in a plastic container for 10 minutes. The resin mixture corresponds to all the other components of the resin composition except the coupling agent and the siloxane compound.
　表１に示す２種類のアモルファス系鉄粉を、加圧式２軸ニーダー（日本スピンドル製造株式会社製、容量５Ｌ）で５分間均一に混合して、金属粉を調製した。表１に示すカップリング剤、及びシロキサン化合物を２軸ニーダー内の金属粉へ添加した。続いて、２軸ニーダーの内容物を９０℃になるまで加熱し、その温度を保持しながら、２軸ニーダーの内容物を１０分間混合した。続いて、上記の樹脂混合物を２軸ニーダーの内容物へ添加して、内容物の温度を１２０℃に保持しながら、内容物を１５分間溶融・混練した。以上の溶融・混練によって得られた混練物を室温まで冷却した後、混練物が所定の粒度を有するようになるまで混練物をハンマーで粉砕した。なお、上記の「溶融」とは、２軸ニーダーの内容物のうち樹脂組成物の少なくとも一部の溶融を意味する。コンパウンド中の金属粉は、コンパウンドの調製過程において溶融しない。以上の方法により、実施例のコンパウンドを調製した。 The two types of amorphous iron powder shown in Table 1 were uniformly mixed for 5 minutes with a pressurized twin-screw kneader (manufactured by Nihon Spindle Manufacturing Co., Ltd., capacity 5 L) to prepare a metal powder. The coupling agent shown in Table 1 and the siloxane compound were added to the metal powder in the biaxial kneader. Subsequently, the contents of the twin-screw kneader were heated to 90 ° C., and the contents of the twin-screw kneader were mixed for 10 minutes while maintaining the temperature. Subsequently, the above 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. After cooling the kneaded product obtained by the above melting and kneading to room temperature, the kneaded product was crushed with a hammer until the kneaded product had a predetermined particle size. The above-mentioned "melting" means melting at least a part of the resin composition in the contents of the twin-screw kneader. The metal powder in the compound does not melt during the compound preparation process. The compound of the example was prepared by the above method.
（比較例）
　分散剤を用いず、金属粉の配合量を表１に示すように変更したこと以外は実施例と同様に操作して、比較例のコンパウンドを調製した。 (Comparative example)
The compound of the comparative example was prepared by operating in the same manner as in the examples except that the compounding amount of the metal powder was changed as shown in Table 1 without using the dispersant.
［コンパウンドの評価］
　実施例及び比較例で得られたコンパウンドについて、以下の評価を行った。結果を表１に示す。 [Compound evaluation]
The compounds obtained in Examples and Comparative Examples were evaluated as follows. The results are shown in Table 1.
（流動特性：１４０℃最低溶融粘度）
　下記のように、１４０℃におけるコンパウンドの最低溶融粘度（単位：Ｐａ・ｓ）を測定した。測定装置としては、株式会社島津製作所製のＣＦＴ‐１００（フローテスター）を用いた。測定用試料として、７ｇのコンパウンドから、タブレットを作製した。１４０℃、２０秒の余熱、１００ｋｇの荷重の条件下で、コンパウンドの流動性を評価した。コンパウンドの流動が停止するまでのプランジャーの押し込み距離（単位：ｍｍ）を、フローテスターストロークとして測定した。コンパウンドの流動が停止するまでの時間を、フロータイムとして測定した。これらの測定値を流動性の指標とした。 (Flow characteristics: 140 ° C minimum melt viscosity)
As shown below, the minimum melt viscosity (unit: Pa · s) of the compound at 140 ° C. was measured. As a measuring device, CFT-100 (flow tester) manufactured by Shimadzu Corporation was used. As a sample for measurement, a tablet was prepared from 7 g of the compound. The fluidity of the compound was evaluated under the conditions of 140 ° C., residual heat for 20 seconds and a load of 100 kg. The pushing distance (unit: mm) of the plunger until the flow of the compound stopped was measured as a flow tester stroke. The time until the flow of the compound stopped was measured as the flow time. These measured values were used as an index of liquidity.
（流動特性：１４０℃円板フロー）
　測定用試料として、５ｇのコンパウンド（粉末）を用いた。コンパウンドを、下型の平坦な表面に置いた。平坦な上型をコンパウンドに押し当てて、コンパウンドを上型及び下型で挟み込んだ。８ｋｇの荷重で３６０秒間、上型及び下型の間のコンパウンドを圧縮することにより、コンパウンドからなる略円板状の成型体を形成した。圧縮中のコンパウンドの温度は、１４０℃に維持された。円板状の成型体の最大径及び最小径を測定した。長径及び短径の平均値が、円板フロー（単位：ｍｍ）に相当する。 (Flow characteristics: 140 ° C disk flow)
As a sample for measurement, 5 g of a compound (powder) was used. The compound was placed on the flat surface of the lower mold. A flat upper mold was pressed against the compound and the compound was sandwiched between the upper and lower molds. By compressing the compound between the upper mold and the lower mold with a load of 8 kg for 360 seconds, a substantially disk-shaped molded body made of the compound was formed. The temperature of the compound during compression was maintained at 140 ° C. The maximum diameter and the minimum diameter of the disk-shaped molded body were measured. The average value of the major axis and the minor axis corresponds to the disk flow (unit: mm).
Figure JPOXMLDOC01-appb-T000001
 
Figure JPOXMLDOC01-appb-T000001
 

Claims (7)

  1. 　金属粉と、エポキシ樹脂、硬化剤及び分散剤を含有する樹脂組成物と、を含み、
    　前記金属粉の含有量が、９０質量％以上９８質量％以下であり、
    　前記分散剤が、リン酸エステルを含む、コンパウンド。     Containing a metal powder and a resin composition containing an epoxy resin, a curing agent and a dispersant,
    The content of the metal powder is 90% by mass or more and 98% by mass or less.
    A compound in which the dispersant comprises a phosphate ester.
  2. 　前記リン酸エステルが、－ＯＲ（Ｒは炭素数４以上の有機基を示す）で表される基を有する、請求項１に記載のコンパウンド。 The compound according to claim 1, wherein the phosphoric acid ester has a group represented by -OR (R indicates an organic group having 4 or more carbon atoms).
  3. 　前記有機基が、炭素数４以上のアルキル基、又は炭素数４以上のアルキル基中の炭素－炭素結合の少なくとも一部にエーテル結合が挿入された基である、請求項２に記載のコンパウンド。 The compound according to claim 2, wherein the organic group is an alkyl group having 4 or more carbon atoms or a group in which an ether bond is inserted into at least a part of a carbon-carbon bond in an alkyl group having 4 or more carbon atoms.
  4. 　前記アルキル基、及びアルキル基中の炭素－炭素結合の少なくとも一部にエーテル結合が挿入された前記基が置換基を有する、請求項３に記載のコンパウンド。 The compound according to claim 3, wherein the alkyl group and the group in which an ether bond is inserted into at least a part of a carbon-carbon bond in the alkyl group have a substituent.
  5. 　前記分散剤の含有量が、前記金属粉１００質量部に対して１質量部以下である、請求項１～４のいずれか一項に記載のコンパウンド。 The compound according to any one of claims 1 to 4, wherein the content of the dispersant is 1 part by mass or less with respect to 100 parts by mass of the metal powder.
  6. 　請求項１～５のいずれか一項に記載のコンパウンドを含む、成型体。 A molded body containing the compound according to any one of claims 1 to 5.
  7. 　請求項１～５のいずれか一項に記載のコンパウンドの硬化物。

          The cured product of the compound according to any one of claims 1 to 5.
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