WO2018096601A1 - Bobine pour machine électrique tournante ainsi que procédé de fabrication de celle-ci, bande de mica, objet durci de bande de mica, et article avec couche isolante - Google Patents

Bobine pour machine électrique tournante ainsi que procédé de fabrication de celle-ci, bande de mica, objet durci de bande de mica, et article avec couche isolante Download PDF

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Publication number
WO2018096601A1
WO2018096601A1 PCT/JP2016/084675 JP2016084675W WO2018096601A1 WO 2018096601 A1 WO2018096601 A1 WO 2018096601A1 JP 2016084675 W JP2016084675 W JP 2016084675W WO 2018096601 A1 WO2018096601 A1 WO 2018096601A1
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WO
WIPO (PCT)
Prior art keywords
mica
mica tape
insulating layer
coil
epoxy compound
Prior art date
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Ceased
Application number
PCT/JP2016/084675
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English (en)
Japanese (ja)
Inventor
みゆき 室町
竹澤　由高
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Resonac Corp
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Hitachi Chemical Co Ltd
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Publication date
Application filed by Hitachi Chemical Co Ltd filed Critical Hitachi Chemical Co Ltd
Priority to PCT/JP2016/084675 priority Critical patent/WO2018096601A1/fr
Priority to JP2018552307A priority patent/JPWO2018096601A1/ja
Publication of WO2018096601A1 publication Critical patent/WO2018096601A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B17/00—Insulators or insulating bodies characterised by their form
    • H01B17/56—Insulating bodies
    • H01B17/60—Composite insulating bodies
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B3/00—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties
    • H01B3/18—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of organic substances
    • H01B3/30—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of organic substances plastics; resins; waxes
    • H01B3/40—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of organic substances plastics; resins; waxes epoxy resins
    • H—ELECTRICITY
    • H02—GENERATION; CONVERSION OR DISTRIBUTION OF ELECTRIC POWER
    • H02K—DYNAMO-ELECTRIC MACHINES
    • H02K3/00—Details of windings
    • H02K3/30—Windings characterised by the insulating material

Definitions

  • the present invention relates to a rotating electrical machine coil, a manufacturing method of a rotating electrical machine coil, mica tape, a cured product of mica tape, and an article with an insulating layer.
  • a coil (hereinafter also simply referred to as a coil) used in a rotating electrical machine such as a generator or an electric motor generally has a coil conductor and an insulating layer disposed on the outer periphery of the coil conductor to insulate the coil conductor from the external environment. is doing.
  • a material for forming the insulating layer an insulating material containing mica called a mica tape is known.
  • the main purpose of the insulating layer formed using mica tape is to electrically insulate the coil from the outside, but the generator adopts an indirect cooling method in which hydrogen gas or air is cooled outside the coil. In these fields, it is desired to increase the thermal conductivity of the insulating layer.
  • a technique for increasing the thermal conductivity of an insulating layer formed using a mica tape a technique for adding an inorganic filler to the mica tape is known.
  • Patent Document 1 describes a mica tape that can form an insulating layer having excellent thermal conductivity by containing alumina having high thermal conductivity as an inorganic filler.
  • an object of the present invention is to provide a coil for a rotating electrical machine having an insulating layer with excellent thermal conductivity and a method for manufacturing the same.
  • Another object of the present invention is to provide a mica tape capable of forming an insulating layer having excellent thermal conductivity, a cured product of the mica tape, and an article with an insulating layer using the same.
  • ⁇ 3> a step of arranging a mica tape containing mica and a resin component on the outer periphery of the coil conductor; Forming an insulating layer from the mica tape disposed on the outer periphery of the coil conductor, and the resin component includes an epoxy compound having a mesogenic structure, according to ⁇ 1> or ⁇ 2> Of manufacturing a coil.
  • a mica tape having a mica layer containing mica and a backing layer containing a backing material and containing a resin component containing an epoxy compound having a mesogenic structure.
  • the epoxy compound having a mesogen structure includes an epoxy compound having two or more mesogen structures and having a number average molecular weight of 600 to 2500 in gel permeation chromatography (GPC) measurement, The listed mica tape.
  • the mica tape according to ⁇ 4> or ⁇ 5>, wherein the epoxy compound having a mesogenic structure includes an epoxy compound having a structure represented by the following general formula (I).
  • R 1 to R 4 each independently represents a hydrogen atom or an alkyl group having 1 to 3 carbon atoms.
  • An article with an insulating layer comprising: an insulator; and an insulating layer that is a cured product of the mica tape according to ⁇ 8>, which is disposed on at least a part of the surface of the insulator.
  • a coil for a rotating electrical machine having a coil conductor and an insulating layer disposed on an outer periphery of the coil conductor, wherein the insulating layer is a cured product of the mica tape according to ⁇ 8>.
  • ⁇ 11> A step of disposing the mica tape according to any one of ⁇ 4> to ⁇ 7> on the outer periphery of the coil conductor, and a step of forming an insulating layer from the mica tape disposed on the outer periphery of the coil conductor And a method for manufacturing a coil for a rotating electrical machine.
  • a coil for a rotating electrical machine having an insulating layer excellent in thermal conductivity and a method for manufacturing the same are provided.
  • goods with an insulating layer using the same are provided.
  • the term “process” includes a process that is independent of other processes and includes the process if the purpose of the process is achieved even if it cannot be clearly distinguished from the other processes. It is.
  • numerical values indicated by using “to” include numerical values described before and after “to” as the minimum value and the maximum value, respectively.
  • the upper limit value or the lower limit value described in one numerical range may be replaced with the upper limit value or the lower limit value of another numerical range. Good. Further, in the numerical ranges described in this specification, the upper limit value or the lower limit value of the numerical range may be replaced with the values shown in the examples.
  • the content rate or content of each component in the composition is such that when there are a plurality of substances corresponding to each component in the composition, the plurality of kinds present in the composition unless otherwise specified. It means the total content or content of substances.
  • the particle diameter of each component in the composition is a mixture of the plurality of types of particles present in the composition unless there is a specific indication when there are a plurality of types of particles corresponding to each component in the composition. Means the value of.
  • the term “layer” refers to the case where the layer is formed only in a part of the region in addition to the case where the layer is formed over the entire region. Is also included.
  • the term “lamination” indicates that layers are stacked, and two or more layers may be combined, or two or more layers may be detachable.
  • the “epoxy compound” means a compound having an epoxy group in the molecule.
  • Epoxy resin is a concept that captures a plurality of epoxy compounds as an aggregate.
  • the “resin component” is a concept including an epoxy resin and a component used as a curing agent as necessary.
  • the coil for a rotating electrical machine of the present embodiment includes a coil conductor and an insulating layer disposed on the outer periphery of the coil conductor, the insulating layer including mica and a cured resin component, and the resin component has a mesogenic structure.
  • the insulating layer includes a cured resin component including an epoxy compound having a mesogenic structure.
  • This insulating layer is superior in thermal conductivity to a conventional insulating layer formed using a resin component containing an epoxy compound having no mesogenic structure.
  • a smectic structure is formed in the cured resin component contained in the insulating layer. Details of the smectic structure will be described later.
  • the insulating layer of the coil for a rotating electrical machine of the present embodiment is formed using, for example, the mica tape of the present embodiment described later.
  • the material, shape, size, and the like of the coil conductor used for the coil of this embodiment are not particularly limited, and can be selected according to the use of the coil.
  • the method for manufacturing a coil for a rotating electrical machine includes a step of placing a mica tape containing mica and a resin component on the outer periphery of a coil conductor, and forming an insulating layer from the mica tape arranged on the outer periphery of the coil conductor.
  • the resin component contains an epoxy compound having a mesogenic structure.
  • the mica tape used in the method for manufacturing a coil for a rotating electrical machine of the present embodiment for example, the mica tape of the present embodiment described later can be used.
  • the method for disposing the mica tape on the outer periphery of the coil conductor is not particularly limited, and a commonly performed method can be adopted.
  • a mica tape is spirally wound around the outer periphery of a coil conductor so that a part of the mica tape overlaps.
  • the thickness of the insulating layer obtained can be adjusted by the number of times the mica tape is wound.
  • the method for forming the insulating layer from the mica tape disposed on the outer periphery of the coil conductor is not particularly limited.
  • the mica tape placed on the outer periphery of the coil conductor is heated while being pressed (heat press), and the resin component contained in the mica tape is allowed to flow out of the mica tape so as to fill the space between the overlapping mica tapes. And a method of curing this to form an insulating layer.
  • the mica tape of the present embodiment includes a mica layer containing mica and a backing layer containing a backing material, and includes a resin component containing an epoxy compound having a mesogenic structure.
  • the resin component containing an epoxy compound having a mesogenic structure tends to have a higher thermal conductivity in a cured state than a resin component containing an epoxy compound not having a mesogenic structure. For this reason, the insulating layer excellent in thermal conductivity can be formed by using the mica tape of this embodiment.
  • the mica tape of the present embodiment cures the resin component contained in the mica tape in a state where the mica tape is disposed on an insulator such as a coil conductor (an object on which an insulating layer is formed on the outer periphery). It is used as a band-like object (also referred to as a prepreg mica tape, RR (Resin Rich) tape, etc.) used for forming an insulating layer on the outer periphery of the insulator.
  • an insulator such as a coil conductor (an object on which an insulating layer is formed on the outer periphery).
  • RR Resin Rich
  • the resin component is present (impregnated) in the mica tape so as to fill at least part of voids inside the mica layer and the backing layer (portions where the mica and the backing material do not exist).
  • the resin component may further exist outside the mica layer and the backing layer.
  • the resin component is not particularly limited as long as it contains an epoxy compound having a mesogenic structure.
  • an epoxy compound having a mesogen structure may be included, or an epoxy compound that does not correspond to an epoxy compound having a mesogen structure may be further included.
  • the proportion of the epoxy compound having a mesogenic structure in the entire epoxy compound (epoxy resin) is preferably 50% by mass or more, and more preferably 70% by mass or more. More preferably, it is 90% by mass or more.
  • the epoxy compound having a mesogenic structure may be one type or two or more types.
  • the mesogenic structure of the epoxy compound include, for example, a biphenyl structure, a phenylbenzoate structure, an azobenzene structure, a stilbene structure, a terphenyl structure, an anthracene structure, a derivative thereof, and two or more of these mesogenic structures via a bonding group. Examples include bonded structures.
  • the epoxy compound having a mesogenic structure preferably exhibits a higher-order structure in a cured state.
  • the higher order structure means a structure including a higher order structure in which constituent elements are arranged to form a micro ordered structure, and corresponds to, for example, a crystal phase and a liquid crystal phase.
  • the presence or absence of such a higher order structure can be determined by a polarizing microscope. That is, in the observation in the crossed Nicols state, it can be distinguished by seeing interference fringes due to depolarization.
  • This higher order structure usually exists in an island shape in the cured product to form a domain structure, and one of the islands corresponds to one higher order structure.
  • the constituent elements of this higher order structure are formed by covalent bonds.
  • Examples of the higher order structure formed in the cured state include a nematic structure and a smectic structure.
  • Each of the nematic structure and the smectic structure is a kind of liquid crystal structure.
  • the nematic structure is a liquid crystal structure in which the molecular long axis is oriented in a uniform direction and has only an alignment order.
  • the smectic structure is a liquid crystal structure having a one-dimensional positional order in addition to the orientation order and having a layer structure. The order is higher in the smectic structure than in the nematic structure.
  • the epoxy compound having a mesogenic structure is more preferably a smectic structure in a cured state.
  • Whether or not a smectic structure is formed in a cured state can be determined by X-ray diffraction measurement of the cured product.
  • X-ray diffraction measurement can be performed, for example, using an X-ray diffraction apparatus manufactured by Rigaku Corporation.
  • the epoxy compound having a mesogenic structure has two or more mesogenic structures and has a number average molecular weight of 600 in gel permeation chromatography (GPC) measurement. It is preferable to include an epoxy compound of ⁇ 2500 (hereinafter also referred to as a specific epoxy compound).
  • the epoxy compound having a mesogenic structure contains a specific epoxy compound
  • the crystallization of the resin component is suppressed and the impregnation property to the mica layer and the backing layer is smaller than when the epoxy compound having a mesogenic structure does not contain the specific epoxy compound.
  • generation of voids in the insulating layer formed using the mica tape is suppressed, and the thermal conductivity tends to be further improved.
  • the number average molecular weight of the specific epoxy compound in gel permeation chromatography (GPC) measurement is preferably 800 to 2000, and more preferably 1000 to 1800.
  • the number average molecular weight of the specific epoxy compound is 800 or more, the impregnation property of the resin component tends to be further improved.
  • the number average molecular weight of the specific epoxy compound is 2000 or less, the crosslinking point density for curing is sufficient. It is ensured and the thermal conductivity tends to be maintained well.
  • the number average molecular weight in the gel permeation chromatography (GPC) measurement of the entire epoxy compound including the specific epoxy compound is preferably 300 to 1500, and more preferably 450 to 1000.
  • the number average molecular weight of an epoxy compound shall be measured on the following measuring conditions.
  • the specific epoxy compound is a compound (hereinafter also referred to as a multimer) obtained by reacting two or more epoxy compounds having the same mesogenic structure as that contained in the specific epoxy compound (hereinafter also referred to as an epoxy monomer). It may be. In this case, even if the specific epoxy compound is obtained by reacting an epoxy monomer with a compound having a functional group capable of reacting with the epoxy group of the epoxy monomer, it is obtained by self-polymerization of the epoxy monomer. Also good.
  • the specific epoxy compound is a multimer obtained by a reaction between an epoxy monomer and a compound having a functional group capable of reacting with an epoxy group of the epoxy monomer
  • the specific epoxy compound includes the following general formula (A) or (B An epoxy compound having a structure represented by:
  • * represents a bonding position with an adjacent atom.
  • Adjacent atoms include oxygen and nitrogen atoms.
  • R 1 to R 3 each independently represents an alkyl group having 1 to 8 carbon atoms.
  • n, m and l each independently represents an integer of 0 to 4.
  • n, m and l are each independently preferably an integer of 0 to 2, more preferably an integer of 0 to 1, and even more preferably 0.
  • the structure represented by the general formula (A) or (B) is preferable.
  • the specific epoxy compound having such a structure tends to have a linear molecular structure. For this reason, it is considered that the stacking property of molecules is high and higher-order structures are more easily formed.
  • R 1 ⁇ R 3, n, m and l are * in formula (A) and (B), R 1 ⁇ R 3, n, The definition and preferred examples of m and l are the same.
  • the specific epoxy compound is an epoxy compound having a structure represented by the general formula (A) or (B)
  • the specific epoxy compound includes an epoxy compound represented by the following general formula (C) or (D). Can be mentioned.
  • R 1 ⁇ R 3 , n, m and l have the general formula (A) and (B) in the R 1 ⁇ R 3, n, m and l Definitions and preferred examples are the same.
  • Ms independently represents a divalent group having a mesogenic structure.
  • Each X independently represents —O— or —NH—.
  • the epoxy compound having a mesogenic structure may be an epoxy compound having a structure represented by the following general formula (I).
  • the resin component containing the epoxy compound having the structure represented by the general formula (I) has a higher glass transition temperature of the obtained cured product and excellent heat resistance than the resin component containing the epoxy compound having another mesogenic structure. There is a tendency. Furthermore, the resin component containing the epoxy compound having the structure represented by the general formula (I) exhibits excellent molecular orientation as compared with other resin components containing the epoxy compound having the mesogenic structure, and such a compound. Tends to have a relatively low melting point and excellent impregnation properties.
  • R 1 to R 4 each independently represents a hydrogen atom or an alkyl group having 1 to 3 carbon atoms.
  • R 1 to R 4 are each independently preferably a hydrogen atom or an alkyl group having 1 to 2 carbon atoms, more preferably a hydrogen atom or a methyl group, and even more preferably a hydrogen atom.
  • 2 to 4 of R 1 to R 4 are hydrogen atoms, more preferably 3 or 4 are hydrogen atoms, and more preferably that all 4 are hydrogen atoms.
  • any of R 1 to R 4 is an alkyl group having 1 to 3 carbon atoms
  • at least one of R 1 and R 4 is preferably an alkyl group having 1 to 3 carbon atoms.
  • the epoxy compound having a structure represented by the general formula (I) is an epoxy compound having at least one selected from the group consisting of structural units represented by the following general formulas (II-A) to (II-D) It may be.
  • R 1 to R 4 each independently represents a hydrogen atom or an alkyl group having 1 to 3 carbon atoms
  • R 5 and R 6 each independently represent carbon.
  • n and m each independently represents an integer of 0 to 4.
  • Each X independently represents —O— or —NH—.
  • R 1 to R 4 in general formulas (II-A) to (II-D) are the same as the specific examples of R 1 to R 4 in general formula (I), and preferred ranges thereof are also the same. .
  • R 5 and R 6 each independently represents an alkyl group having 1 to 8 carbon atoms, preferably an alkyl group having 1 to 3 carbon atoms, More preferably, it is a group.
  • n and m each independently represent an integer of 0 to 4, preferably an integer of 0 to 2, and preferably an integer of 0 to 1. Is more preferred and 0 is even more preferred. That is, the benzene ring to which R 5 or R 6 is attached in the general formulas (II-A) to (II-D) preferably has 2 to 4 hydrogen atoms, and preferably 3 or 4 hydrogen atoms. More preferably, it has an atom, and further preferably has 4 hydrogen atoms.
  • R 1 ⁇ R 6 in the general formula (II-a) ⁇ (II -d), n, definition and preferred examples of m and X have the general formula (II-A) ⁇ (II -D) in R 1 ⁇ R 6 , the same as the definition and preferred examples of n, m and X.
  • the epoxy compound having the structure represented by the general formula (I) is an epoxy compound (dimer) containing two structural units represented by the general formula (I), the following general formula ( Examples thereof include at least one selected from the group consisting of epoxy compounds represented by III-A) to (III to F).
  • Formula (III-A) ⁇ R 1 in (III ⁇ F) ⁇ R 6 , n, the definition of m and X have the general formula (II-A) R 1 in the ⁇ (II-D) ⁇ R 6, n , M and X are the same, and the preferred range is also the same.
  • Formula (III-a) ⁇ R 1 in (III ⁇ f) ⁇ R 6 , n, the definition of m and X have the general formula (III-A) R 1 in the ⁇ (III-F) ⁇ R 6, n , M and X are the same, and the preferred range is also the same.
  • a method for synthesizing a multimer by reacting an epoxy monomer with a compound having a functional group capable of reacting with an epoxy group of the epoxy monomer is not particularly limited. Specifically, for example, by dissolving an epoxy monomer, a compound having a functional group capable of reacting with an epoxy group of the epoxy monomer, and a reaction catalyst used as necessary in a solvent, stirring while heating, Multimers can be synthesized. Alternatively, for example, an epoxy monomer and a compound having a functional group capable of reacting with an epoxy group of the epoxy monomer are mixed without using a reaction catalyst and a solvent, if necessary, and stirred while heating to produce a multimer. Can be synthesized.
  • Examples of the epoxy monomer include an epoxy compound having a mesogenic structure represented by the following general formula (M).
  • the resin component containing the epoxy compound represented by the general formula (M) forms a smectic liquid crystal structure in the cured product.
  • an epoxy monomer contains the epoxy compound represented by general formula (M)
  • only 1 type may be sufficient as the epoxy compound represented by general formula (M), or 2 or more types may be sufficient as it.
  • R 1 to R 4 each independently represents a hydrogen atom or an alkyl group having 1 to 3 carbon atoms.
  • R 1 to R 4 are each independently preferably a hydrogen atom or an alkyl group having 1 to 2 carbon atoms, more preferably a hydrogen atom or a methyl group, and even more preferably a hydrogen atom.
  • 2 to 4 of R 1 to R 4 are hydrogen atoms, more preferably 3 or 4 are hydrogen atoms, and more preferably that all 4 are hydrogen atoms.
  • any of R 1 to R 4 is an alkyl group having 1 to 3 carbon atoms
  • at least one of R 1 and R 4 is preferably an alkyl group having 1 to 3 carbon atoms.
  • the solvent is not particularly limited as long as it can dissolve the epoxy monomer and the compound having a functional group capable of reacting with the epoxy group of the epoxy monomer and can be heated to a temperature necessary for the reaction of both compounds.
  • Specific examples include cyclohexanone, cyclopentanone, ethyl lactate, propylene glycol monomethyl ether, N-methylpyrrolidone and the like.
  • the amount of the solvent is not particularly limited as long as it is an amount capable of dissolving the epoxy monomer, the compound having a functional group capable of reacting with the epoxy group of the epoxy monomer, and the reaction catalyst used as necessary at the reaction temperature.
  • solubility differs depending on the type of raw material before the reaction, the type of solvent, etc., for example, if the charged solid content concentration is 20% by mass to 60% by mass, the viscosity of the solution after the reaction is in a preferred range. There is a tendency.
  • the compound having a functional group capable of reacting with the epoxy group of the epoxy monomer is not particularly limited. From the viewpoint of forming a smectic structure in the cured product, a compound having a functional group capable of reacting with an epoxy group of an epoxy monomer is a dihydroxybenzene compound having a structure in which two hydroxyl groups are bonded to one benzene ring, and two amino groups.
  • a diaminobenzene compound having a structure in which a group is bonded to one benzene ring, a dihydroxybiphenyl compound having a structure in which one hydroxyl group is bonded to each of two benzene rings forming a biphenyl structure, and two benzene rings forming a biphenyl structure It is preferably at least one selected from the group consisting of diaminobiphenyl compounds each having a structure in which one amino group is bonded (hereinafter also referred to as a specific aromatic compound).
  • a multimer having at least one selected from the group consisting of structures represented by general formulas (IA) to (ID) by reacting an epoxy group of an epoxy monomer with a hydroxyl group or an amino group of a specific aromatic compound Can be synthesized.
  • Examples of the dihydroxybenzene compound include 1,2-dihydroxybenzene (catechol), 1,3-dihydroxybenzene (resorcinol), 1,4-dihydroxybenzene (hydroquinone), and derivatives thereof.
  • Examples of the diaminobenzene compound include 1,2-diaminobenzene, 1,3-diaminobenzene, 1,4-diaminobenzene, and derivatives thereof.
  • Examples of the dihydroxybiphenyl compound include 3,3′-dihydroxybiphenyl, 3,4′-dihydroxybiphenyl, 4,4′-dihydroxybiphenyl, and derivatives thereof.
  • Examples of the diaminobiphenyl compound include 3,3′-diaminobiphenyl, 3,4′-diaminobiphenyl, 4,4′-diaminobiphenyl, and derivatives thereof.
  • Examples of the derivative of the specific aromatic compound include a compound in which a substituent such as an alkyl group having 1 to 8 carbon atoms is bonded to the benzene ring of the specific aromatic compound.
  • a specific aromatic compound may be used individually by 1 type, and may use 2 or more types together.
  • the specific aromatic compounds include 1,4-dihydroxybenzene, 1,4-diaminobenzene, 4,4′-dihydroxybiphenyl and 4,4. '-Diaminobiphenyl is preferred.
  • the multimer obtained by reacting them with an epoxy monomer tends to have a linear structure. For this reason, it is considered that the stacking property of the molecule is high and it is easy to form a smectic structure in the cured product.
  • reaction catalyst is not particularly limited, and an appropriate one can be selected from the viewpoint of reaction rate, reaction temperature, storage stability, and the like. Specific examples include imidazole compounds, organophosphorus compounds, tertiary amines, and quaternary ammonium salts.
  • a reaction catalyst may be used individually by 1 type, and may use 2 or more types together.
  • an organic phosphorus compound is preferable as the reaction catalyst.
  • the organic phosphorus compound include an organic phosphine compound, a compound having an intramolecular polarization formed by adding a compound having a ⁇ bond such as maleic anhydride, a quinone compound, diazophenylmethane, and a phenol resin to an organic phosphine compound, organic And a complex of a phosphine compound and an organic boron compound.
  • organic phosphine compound examples include triphenylphosphine, diphenyl (p-tolyl) phosphine, tris (alkylphenyl) phosphine, tris (alkoxyphenyl) phosphine, tris (alkylalkoxyphenyl) phosphine, tris (dialkylphenyl) phosphine, Tris (trialkylphenyl) phosphine, tris (tetraalkylphenyl) phosphine, tris (dialkoxyphenyl) phosphine, tris (trialkoxyphenyl) phosphine, tris (tetraalkoxyphenyl) phosphine, trialkylphosphine, dialkylarylphosphine, alkyldiaryl A phosphine etc. are mentioned.
  • quinone compound examples include 1,4-benzoquinone, 2,5-toluquinone, 1,4-naphthoquinone, 2,3-dimethylbenzoquinone, 2,6-dimethylbenzoquinone, 2,3-dimethoxy-5-methyl- Examples include 1,4-benzoquinone, 2,3-dimethoxy-1,4-benzoquinone, and phenyl-1,4-benzoquinone.
  • organic boron compound examples include tetraphenyl borate, tetra-p-tolyl borate, and tetra-n-butyl borate.
  • the amount of the reaction catalyst is not particularly limited. From the viewpoint of reaction rate and storage stability, 0.1 to 1.5 parts by mass with respect to 100 parts by mass of the total of the epoxy monomer and the compound having a functional group capable of reacting with the epoxy group of the epoxy monomer. Preferably, the amount is 0.2 to 1 part by mass.
  • all of the epoxy monomers may react to form a multimer, or a part of the epoxy monomer may remain unreacted in the monomer state. .
  • Multimer synthesis can be performed using a reaction vessel such as a flask for a small scale and a synthesis kettle for a large scale.
  • a specific synthesis method is as follows, for example. First, an epoxy monomer is put into a reaction vessel, a solvent is put in if necessary, and heated to a reaction temperature with an oil bath or a heat medium to dissolve the epoxy monomer. A compound having a functional group capable of reacting with the epoxy group of the epoxy monomer is added thereto, and then a reaction catalyst is introduced as necessary to start the reaction. Subsequently, a multimer is obtained by distilling a solvent off under reduced pressure as needed.
  • the reaction temperature is not particularly limited as long as the reaction between the epoxy group of the epoxy monomer and the functional group capable of reacting with the epoxy group proceeds, and is preferably in the range of 100 ° C. to 180 ° C., for example, More preferably, it is in the range of ⁇ 150 ° C.
  • the reaction temperature is set to 100 ° C. or higher, the time until the reaction is completed tends to be shortened.
  • the reaction temperature to 180 ° C. or lower, the possibility of gelation tends to be reduced.
  • the compounding ratio of the epoxy monomer used for the synthesis of the multimer and the compound having a functional group capable of reacting with the epoxy group of the epoxy monomer is not particularly limited.
  • the blending ratio in which the ratio (A: B) of the number of equivalents of epoxy groups (A) to the number of equivalents of functional groups capable of reacting with epoxy groups (A: B) is in the range of 100: 100 to 100: 1.
  • A: B is in the range of 100: 50 to 100: 1 is preferable.
  • the structure of the multimer is, for example, the molecular weight of the multimer estimated from the reaction between the epoxy monomer used for the synthesis and a compound having a functional group capable of reacting with the epoxy group of the epoxy monomer, UV, and mass spectrum. It can be determined by collating the molecular weight of the target compound determined by liquid chromatography carried out using a liquid chromatograph equipped with a detector.
  • the ratio of the multimer to the entire epoxy compound is preferably 10% by mass or more, more preferably 20% by mass or more, and more preferably 30% by mass or more of the entire epoxy compound. Is more preferable.
  • the content is preferably 80% by mass or less, more preferably 75% by mass or less, and further preferably 70% by mass or less based on the entire epoxy compound.
  • the proportion of the dimer in the entire epoxy compound is not particularly limited.
  • the content of the dimer is preferably 10% by mass or more of the entire epoxy compound, more preferably 15% by mass or more, and further preferably 20% by mass or more.
  • the content of the dimer is preferably 60% by mass or less, more preferably 55% by mass or less, and further preferably 50% by mass or less of the entire epoxy compound. .
  • the ratio of the epoxy monomer in the entire epoxy compound is not particularly limited.
  • the content of the epoxy monomer is preferably 30% by mass or more of the entire epoxy compound, more preferably 35% by mass or more, and further preferably 40% by mass or more.
  • the content of the epoxy monomer is preferably 90% by mass or less, more preferably 80% by mass or less, and further preferably 70% by mass or less, based on the entire epoxy compound.
  • the epoxy compound includes an epoxy compound having a mesogenic structure (epoxy monomer) and an epoxy compound having two or more mesogenic structures having the same structure as the mesogenic structure of the epoxy monomer (multimer), from the viewpoint of impregnation
  • the ratio of the epoxy monomer obtained by liquid chromatography is preferably 50% or less of the entire epoxy compound.
  • the resin component in which the proportion of the epoxy monomer obtained by liquid chromatography is 50% or less of the entire epoxy compound tends to be excellent in impregnation properties compared to the resin component in which the proportion of the epoxy monomer exceeds 50% of the entire epoxy resin.
  • the reason is not clear, but when the proportion of the epoxy monomer is 50% or less of the whole epoxy compound, the proportion of multimers having high molecular mobility and relatively low orientation is large in the resin component, This is presumed to be due to higher nature.
  • Liquid chromatography is performed at a sample concentration of 0.5% by mass, tetrahydrofuran as the mobile phase, and a flow rate of 1.0 ml / min.
  • the measurement can be performed using, for example, a high performance liquid chromatograph “L6000” manufactured by Hitachi, Ltd. and a data analysis apparatus “C-R4A” manufactured by Shimadzu Corporation.
  • As the column for example, “G2000HXL” and “G3000HXL” which are GPC columns manufactured by Tosoh Corporation can be used.
  • the proportion of the epoxy monomer obtained by liquid chromatography is preferably 50% or less of the whole epoxy compound, more preferably 49% or less, and 48% or less. Further preferred.
  • the proportion of the epoxy monomer obtained by liquid chromatography is preferably 35% or more of the entire epoxy compound, more preferably 37% or more, and 40% More preferably, it is the above.
  • the kind of mica contained in the mica layer is not particularly limited. Examples include unfired hard mica, fired hard mica, unfired soft mica, fired soft mica, synthetic mica, and flake mica. Among these, unfired hard mica is preferable from the viewpoints of price and availability.
  • the particle size of mica is not particularly limited.
  • the proportion of mica pieces having a particle diameter of 2.8 mm or more is preferably less than 45% by mass of the whole mica pieces, It is more preferably 30% by mass or less, and further preferably 20% by mass or less, based on the entire mica piece.
  • the proportion of mica pieces having a particle diameter of 0.5 mm or more when sieved using a JIS standard sieve is 40% by mass or more of the entire mica pieces. Is preferable, and it is more preferable that it is 60 mass% or more.
  • JIS standard sieve conforms to JIS-Z-8801-1: 2006 and conforms to ISO3310-1: 2000.
  • ISO 3310-1: 2000 it is preferable to apply a sieve having a square shape as in JIS-Z-8801-1: 2006.
  • the ratio of mica pieces having a particle diameter of 2.8 mm or more when sieving using a JIS standard sieve in mica contained in the mica tape, and the ratio of mica pieces having a particle diameter of 0.5 mm or more are, for example, It can be confirmed as follows.
  • methyl ethyl ketone is added to the remaining solid after removing the supernatant, and the mixture is shaken for 10 minutes and then centrifuged at 8000 rpm for 5 minutes. The supernatant is removed, 100 g of methyl ethyl ketone is added to 1 g of the remaining solid, and the mixture is dispersed for 30 minutes with a mix rotor and shaken for another 10 minutes. Then, while shaking the container, JIS standard sieves (JIS-Z-8801-1: 2006, ISO3310-1: 2000, Tokyo Screen Co., Ltd., test sieve) ). The sieving is performed using an electromagnetic sieve vibrator at a frequency of 3000 times / minute, an amplitude of 1 mm, and 10 minutes.
  • JIS standard sieves JIS-Z-8801-1: 2006, ISO3310-1: 2000, Tokyo Screen Co., Ltd., test sieve
  • a mica piece that has not passed through a sieve having an opening of 2.8 mm (or 0.5 mm) is defined as a “mica piece having a particle diameter of 2.8 mm (or 0.5 mm) or more”.
  • the ratio (mass%) of “mica pieces with a particle diameter of 2.8 mm (or 0.5 mm) or more” in the total amount of mica pieces before being divided is “particle diameter when sieving using a JIS standard sieve. Is the ratio of mica pieces with 2.8 mm (or 0.5 mm) or more.
  • Mica may be used alone or in combination of two or more.
  • two or more mica are used in combination, for example, when two or more mica having the same component and different particle sizes are used, when two or more mica having the same particle size and different components are used, and the average particle size and component The case where 2 or more types of mica having different types is used is mentioned.
  • the amount of mica in the mica layer is not particularly limited. For example, a range of 80 g / m 2 to 230 g / m 2 is preferable, and a range of 100 g / m 2 to 200 g / m 2 is more preferable. If the amount of mica in the mica layer is 80 g / m 2 or more, sufficient insulating properties tend to be secured. If the amount of mica in the mica layer is 230 g / m 2 or less, the thickness of the mica tape can be reduced, and sufficient thermal conductivity tends to be ensured.
  • the type of the backing material contained in the backing layer of the mica tape is not particularly limited.
  • a glass cloth is mentioned.
  • the resin component penetrated between the fibers constituting the glass cloth is well integrated with the adjacent mica layer, and the thermal conductivity of the insulating layer tends to be further improved.
  • the average thickness of the backing material is not particularly limited.
  • the thickness is preferably 30 ⁇ m to 60 ⁇ m, and more preferably 45 ⁇ m to 50 ⁇ m.
  • the average thickness of the backing material is 30 ⁇ m or more, it is suppressed that the backing layer becomes too thin following the thickness of the backing material when the mica tape is pressed, and a decrease in thermal conductivity is suppressed. There is a tendency. If the thickness of the backing material is 60 ⁇ m or less, the thickness of the mica tape can be suppressed, and the occurrence of breakage, cracks, and the like of the mica tape during the process of winding the mica tape around the insulator tends to be suppressed.
  • the average thickness of the backing material is determined by measuring the thickness of the backing material at a total of 10 locations using a micrometer (for example, “MDC-SB” manufactured by Mitutoyo Corporation). Arithmetic mean value.
  • the backing material may be surface-treated if necessary.
  • Examples of the surface treatment method for the backing material include treatment with a silane coupling agent.
  • the mica tape may contain other components other than the epoxy resin, mica and the backing material as necessary.
  • examples of other components include a curing catalyst, an inorganic filler, a curing agent, a coupling agent, an antioxidant, an anti-aging agent, a stabilizer, a flame retardant, and a thickener.
  • the content is not particularly limited.
  • the curing catalyst include compounds exemplified as the reaction catalyst that can be used for the synthesis of the above-described multimer of epoxy compounds.
  • the inorganic filler examples include silica, boron nitride and alumina.
  • Alumina is preferable from the viewpoint of thermal conductivity.
  • Boron nitride is preferable from the viewpoint of achieving both thermal conductivity and winding ability of the mica tape.
  • the type of boron nitride is not particularly limited, and examples include hexagonal boron nitride (h-BN), cubic boron nitride (c-BN), and wurtzite boron nitride. Among these, hexagonal boron nitride (h-BN) is preferable.
  • the boron nitride may be primary particles of boron nitride formed in a scale shape or secondary particles formed by agglomeration of primary particles.
  • the average particle size of the inorganic filler is not particularly limited. For example, it is preferably 1 ⁇ m to 40 ⁇ m, more preferably 5 ⁇ m to 20 ⁇ m, and even more preferably 5 ⁇ m to 10 ⁇ m.
  • the average particle diameter of the inorganic filler can be measured by using, for example, a laser diffraction / scattering particle size distribution measuring apparatus (Microtrac MT3000II, Nikkiso Co., Ltd.). Specifically, an inorganic filler is introduced into pure water and then dispersed with an ultrasonic disperser. By measuring the particle size distribution of the dispersion, the particle size distribution of the inorganic filler is measured. Based on this particle size distribution, the particle size (D50) corresponding to 50% volume accumulation from the small diameter side is determined as the average particle size.
  • a laser diffraction / scattering particle size distribution measuring apparatus Microtrac MT3000II, Nikkiso Co., Ltd.
  • the inorganic filler may be used alone or in combination of two or more.
  • two or more inorganic fillers are used in combination, for example, when two or more inorganic fillers having the same component and different average particle sizes are used, two or more inorganic fillers having the same average particle size and different components are used, and A case where two or more inorganic fillers having different average particle diameters and types are used.
  • the curing agent examples include amine curing agents, phenol curing agents, acid anhydride curing agents, polymercaptan curing agents, polyaminoamide curing agents, isocyanate curing agents, and blocked isocyanate curing agents.
  • the average thickness of the mica tape is not particularly limited.
  • the average thickness of the mica tape may be 400 ⁇ m or less, preferably 350 ⁇ m or less, and more preferably 300 ⁇ m or less.
  • the average thickness of the mica tape is preferably 300 ⁇ m or less, and more preferably 290 ⁇ m or less. From the viewpoint of insulation, the average thickness of the mica tape is preferably 120 ⁇ m or more, more preferably 150 ⁇ m or more, and further preferably 160 ⁇ m or more.
  • the average thickness of the mica layer is not particularly limited. From the viewpoint of ease of winding the mica tape, the average thickness of the mica layer is preferably 180 ⁇ m or less, and more preferably 170 ⁇ m or less. From the viewpoint of electrical insulation, the average thickness of the mica layer is preferably 80 ⁇ m or more, and more preferably 90 ⁇ m or more.
  • the average thickness of the backing layer is not particularly limited. From the viewpoint of ease of winding the mica tape, the average thickness of the backing layer is preferably 60 ⁇ m or less, and more preferably 50 ⁇ m or less. From the viewpoint of the strength of the mica tape, the average thickness of the backing layer is preferably 10 ⁇ m or more, and more preferably 20 ⁇ m or more.
  • the average thickness of the mica tape is determined by measuring the thickness of the mica tape at a total of 10 locations using a micrometer (for example, “MDC-SB” manufactured by Mitutoyo Corporation). Arithmetic mean value.
  • the thickness of the mica layer and the backing layer in the mica tape is determined by measuring the thickness of the mica layer and the backing layer in the cross section of the mica tape with a micrometer of a stereomicroscope (for example, Olympus Corporation “BX51”). Observe 3 points and use the arithmetic average.
  • a stereomicroscope for example, Olympus Corporation “BX51”.
  • the content of the resin component in the mica tape is not particularly limited, and can be selected according to the use of the mica tape.
  • the content of the resin component in the mica tape is preferably 15% by mass to 40% by mass, and more preferably 25% by mass to 33% by mass with respect to the entire mica tape.
  • the content rate of the resin component in the mica tape is calculated by the following method, for example.
  • the mica tape cut to a size of 30 mm in width and 50 mm in length is heated in an electric furnace at 600 ° C. for 2 hours, and the mass reduction rate (%) before and after heating is obtained by the following formula.
  • the above process is performed three times, and an arithmetic average value of the obtained values is obtained.
  • Content of resin component ⁇ (mass before heating ⁇ mass after heating) / mass before heating ⁇ ⁇ 100
  • the content of the inorganic filler in the mica tape is not particularly limited.
  • the mica tape may have a protective layer (protective film) provided on the outermost surface of the mica tape, if necessary.
  • ⁇ Mica tape manufacturing method> The manufacturing method in particular of the mica tape of this embodiment is not restrict
  • the mica paper is a sheet-like object formed by gathering mica.
  • the composition may contain a solvent.
  • the solvent By including the solvent, the viscosity of the composition is lowered, and the impregnation property tends to be improved.
  • the type of the solvent is not particularly limited, and can be selected from commonly used organic solvents. Specific examples include cyclohexanone, methyl ethyl ketone, toluene, methanol and the like.
  • a solvent may use only 1 type or may use 2 or more types together.
  • the composition applied to the backing material oozes out to the other surface side (mica paper side) of the backing material and penetrates all or part of the mica paper.
  • the mica paper can easily become independent and is not easily collapsed.
  • the cured product of the mica tape of this embodiment is obtained by curing the resin component contained in the mica tape described above.
  • the curing method is not particularly limited, and can be selected from ordinary methods.
  • the article with an insulating layer according to the present embodiment includes an insulator and an insulating layer that is a cured product of the mica tape according to the present embodiment that is disposed on at least a part of the surface of the insulator.
  • the method for forming the insulating layer using the mica tape of the present embodiment is not particularly limited, and conventionally known production methods can be applied. For example, after winding mica tape around an insulator, heat it while applying pressure to the mica tape (heat press), and let the resin component contained in the mica tape flow out of the mica tape in advance and overlap between the overlapping mica tapes. There is a method of forming an insulating layer by filling and curing the insulating layer.
  • the insulator to be applied to the article with an insulating layer of the present embodiment is not particularly limited, and examples thereof include a coil conductor of a coil for a rotating electrical machine described above, rod-shaped copper, and plate-shaped copper.
  • an insulating layer having excellent thermal conductivity can be formed. Therefore, when the article with an insulating layer of the present embodiment is a coil, when cooling the coil, a hydrogen cooling method or an air cooling method is adopted even for a coil of a scale that conventionally employs a direct water cooling method. It becomes possible to simplify the structure of the coil.
  • hydroquinone was added as a specific aromatic compound.
  • the amount of hydroquinone added was such that the ratio (A: B) of the number of equivalents (A) of epoxy groups of the epoxy compound to the number of equivalents (B) of hydroxyl groups of hydroquinone was 100: 13.
  • 0.5 g of triphenylphosphine was added as a reaction catalyst, and heating was continued at an oil bath temperature of 120 ° C. After continuing the heating for 5 hours, propylene glycol monomethyl ether was distilled off under reduced pressure from the reaction solution, and the residue was cooled to room temperature (25 ° C.), whereby a part of the epoxy compound formed a multimer (prepolymerization). An epoxy resin in a state was obtained.
  • the number average molecular weight of the obtained epoxy resin was measured by gel permeation chromatography (GPC), the number average molecular weight of the component corresponding to the multimer was 1315, and it was confirmed that a specific epoxy compound was produced. It was. Moreover, the number average molecular weight of the whole epoxy resin containing an unreacted epoxy compound was 531. In addition, the number average molecular weight of the epoxy compound before using for the synthesis
  • a glass cloth (Soyo Co., Ltd., “WEA 03G 103”, thickness 0.030 mm) as a backing material is laminated on the mica paper placed on the table, and the resin composition heated to 90 ° C. on the upper surface of the glass cloth.
  • the application was carried out so that the resin composition penetrates the entire mica paper under the glass cloth, and the impregnation property of the resin composition into the glass cloth and mica paper was good.
  • the laminate was dried at 100 ° C. for 20 minutes to produce a laminate comprising a mica layer containing a resin component and a glass cloth layer (backing layer). The laminate was cut so that the width was 30 mm to produce a mica tape.
  • Example 2 Example 1 except that the amount of hydroquinone added was changed so that the ratio (A: B) of the number of equivalents of epoxy groups (A) of the epoxy compound to the number of equivalents (B) of hydroxyl groups of hydroquinone was 100: 25. Thus, an epoxy resin was synthesized.
  • the number average molecular weight of the obtained epoxy resin was measured by gel permeation chromatography (GPC), the number average molecular weight of the component corresponding to the multimer was 1530, and it was confirmed that a specific epoxy compound was produced. It was. Moreover, the number average molecular weight of the whole epoxy resin containing an unreacted epoxy compound was 590.
  • a resin composition was prepared by mixing 97.1% by mass of the synthesized epoxy resin and 2.9% by mass of boron trifluoride monoethylamine (Wako Pure Chemical Industries, Ltd.) as a curing catalyst.
  • Example 3 Similar to Example 1 except that the amount of hydroquinone added was changed so that the ratio (A: B) of the number of equivalents of epoxy groups (A) of the epoxy compound to the number of equivalents of hydroxyl groups (B) of hydroquinone was 100: 30. Thus, an epoxy resin was synthesized.
  • the number average molecular weight of the component corresponding to the multimer was 1610, and it was confirmed that a specific epoxy compound was produced. . Moreover, the number average molecular weight of the whole epoxy resin containing an unreacted epoxy compound was 608.
  • a resin composition was prepared by mixing 97.1% by mass of the synthesized epoxy resin and 2.9% by mass of boron trifluoride monoethylamine (Wako Pure Chemical Industries, Ltd.) as a curing catalyst.
  • the mica tapes of Examples 1 to 3 produced using an epoxy resin containing an epoxy compound having a mesogenic structure were produced using an epoxy resin not containing an epoxy compound having a mesogenic structure.
  • the thermal conductivity after curing was high. From the above, it was found that the mica tape of this embodiment can form an insulating layer having excellent thermal conductivity.

Landscapes

  • Engineering & Computer Science (AREA)
  • Power Engineering (AREA)
  • Physics & Mathematics (AREA)
  • Spectroscopy & Molecular Physics (AREA)
  • Epoxy Resins (AREA)
  • Insulated Conductors (AREA)
  • Insulating Bodies (AREA)
  • Insulation, Fastening Of Motor, Generator Windings (AREA)
  • Manufacture Of Motors, Generators (AREA)

Abstract

L'invention concerne une bobine pour machine électrique tournante qui possède un conducteur de bobine, et une couche isolante disposée à la périphérie dudit conducteur de bobine. Ladite couche isolante contient un mica et un objet durci d'un composant résine. Ledit composant résine contient un composé possédant une structure de mésogène.
PCT/JP2016/084675 2016-11-22 2016-11-22 Bobine pour machine électrique tournante ainsi que procédé de fabrication de celle-ci, bande de mica, objet durci de bande de mica, et article avec couche isolante Ceased WO2018096601A1 (fr)

Priority Applications (2)

Application Number Priority Date Filing Date Title
PCT/JP2016/084675 WO2018096601A1 (fr) 2016-11-22 2016-11-22 Bobine pour machine électrique tournante ainsi que procédé de fabrication de celle-ci, bande de mica, objet durci de bande de mica, et article avec couche isolante
JP2018552307A JPWO2018096601A1 (ja) 2016-11-22 2016-11-22 回転電機用コイル、回転電機用コイルの製造方法、マイカテープ、マイカテープの硬化物及び絶縁層付き物品

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PCT/JP2016/084675 WO2018096601A1 (fr) 2016-11-22 2016-11-22 Bobine pour machine électrique tournante ainsi que procédé de fabrication de celle-ci, bande de mica, objet durci de bande de mica, et article avec couche isolante

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Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2003009446A (ja) * 2001-06-19 2003-01-10 Hitachi Ltd 高熱伝導絶縁コイルおよび回転電機装置
JP4703242B2 (ja) * 2005-04-13 2011-06-15 株式会社日立製作所 電機子巻線
WO2015053374A1 (fr) * 2013-10-09 2015-04-16 日立化成株式会社 Bande de mica préimprégnée et bobine la comprenant
WO2016104772A1 (fr) * 2014-12-26 2016-06-30 日立化成株式会社 Résine époxy, composition de résine époxy, composition de résine époxy contenant une charge inorganique, feuille de résine, produit durci, et composé époxy
WO2016121758A1 (fr) * 2015-01-29 2016-08-04 日立化成株式会社 Composition de résine époxyde, composition de résine époxyde semi-durcie, feuille de résine et préimprégné

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2003009446A (ja) * 2001-06-19 2003-01-10 Hitachi Ltd 高熱伝導絶縁コイルおよび回転電機装置
JP4703242B2 (ja) * 2005-04-13 2011-06-15 株式会社日立製作所 電機子巻線
WO2015053374A1 (fr) * 2013-10-09 2015-04-16 日立化成株式会社 Bande de mica préimprégnée et bobine la comprenant
WO2016104772A1 (fr) * 2014-12-26 2016-06-30 日立化成株式会社 Résine époxy, composition de résine époxy, composition de résine époxy contenant une charge inorganique, feuille de résine, produit durci, et composé époxy
WO2016121758A1 (fr) * 2015-01-29 2016-08-04 日立化成株式会社 Composition de résine époxyde, composition de résine époxyde semi-durcie, feuille de résine et préimprégné

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