WO2012153636A1 - Vernis de résine de polyimide, fil électrique isolé l'utilisant, bobine électrique et moteur - Google Patents

Vernis de résine de polyimide, fil électrique isolé l'utilisant, bobine électrique et moteur Download PDF

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Publication number
WO2012153636A1
WO2012153636A1 PCT/JP2012/061047 JP2012061047W WO2012153636A1 WO 2012153636 A1 WO2012153636 A1 WO 2012153636A1 JP 2012061047 W JP2012061047 W JP 2012061047W WO 2012153636 A1 WO2012153636 A1 WO 2012153636A1
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WIPO (PCT)
Prior art keywords
insulating layer
polyimide resin
polyimide
resin varnish
conductor
Prior art date
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PCT/JP2012/061047
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English (en)
Japanese (ja)
Inventor
吉田　健吾
雅晃 山内
正隆 志波
悠史 畑中
惇一 今井
菅原　潤
清水　亨
齋藤　秀明
雄大 古屋
Original Assignee
住友電工ウインテック株式会社
住友電気工業株式会社
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Application filed by 住友電工ウインテック株式会社, 住友電気工業株式会社 filed Critical 住友電工ウインテック株式会社
Publication of WO2012153636A1 publication Critical patent/WO2012153636A1/fr

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    • 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
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
    • C09D179/00—Coating compositions based on macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing nitrogen, with or without oxygen, or carbon only, not provided for in groups C09D161/00 - C09D177/00
    • C09D179/04—Polycondensates having nitrogen-containing heterocyclic rings in the main chain; Polyhydrazides; Polyamide acids or similar polyimide precursors
    • C09D179/08—Polyimides; Polyester-imides; Polyamide-imides; Polyamide acids or similar polyimide precursors
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
    • C09D5/00—Coating compositions, e.g. paints, varnishes or lacquers, characterised by their physical nature or the effects produced; Filling pastes
    • C09D5/18—Fireproof paints including high temperature resistant paints
    • 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
    • H01B3/303—Macromolecular compounds obtained by reactions forming a linkage containing nitrogen with or without oxygen or carbon in the main chain of the macromolecule, not provided for in groups H01B3/38 or H01B3/302
    • H01B3/306—Polyimides or polyesterimides
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F5/00—Coils
    • H01F5/06—Insulation of windings
    • H—ELECTRICITY
    • H02—GENERATION; CONVERSION OR DISTRIBUTION OF ELECTRIC POWER
    • H02K—DYNAMO-ELECTRIC MACHINES
    • H02K3/00—Details of windings
    • H02K3/04—Windings characterised by the conductor shape, form or construction, e.g. with bar conductors
    • H02K3/18—Windings for salient poles

Definitions

  • the present invention relates to a polyimide resin varnish that can be coated and baked on a conductor to form an insulating film, an insulated wire having an insulating layer formed using this polyimide resin varnish, an electric coil, and a motor using the same.
  • an insulating layer (insulating film) covering the conductor is required to have excellent insulation, adhesion to the conductor, heat resistance, mechanical strength, and the like.
  • the resin forming the insulating layer include polyimide resin, polyamideimide resin, and polyesterimide resin.
  • a high voltage is applied to an insulated wire constituting the electric device, and partial discharge (corona discharge) is likely to occur on the surface of the insulating film.
  • the generation of corona discharge is likely to cause local temperature rise and generation of ozone and ions.
  • Insulated wires used at high voltages are also required to improve the corona discharge starting voltage for the above reasons, and it is known that reducing the dielectric constant of the insulating layer is effective for this purpose.
  • Patent Document 1 discloses an enameled wire in which a polyimide resin enamel film layer is applied and baked directly on a conductor as an enameled wire having a heat resistance class C (class of 180 ° C. or higher).
  • Patent Document 2 describes a polyimide resin having an aromatic ether structure. Specifically, a polyimide by reacting an acid anhydride having an aromatic ether structure such as 4,4′-oxydiphthalic dianhydride (ODPA) with a diamine having an aromatic ether structure and a diamine having a fluorene structure. The precursor is synthesized. The flexibility is improved by using an acid anhydride having an aromatic ether structure and a diamine. Further, it is described that the polyimide resin having such a structure has a low dielectric constant and can provide an insulating film excellent in suppressing corona generation.
  • ODPA 4,4′-oxydiphthalic dianhydride
  • polyimide resin is a material having excellent heat resistance, mechanical properties, and electrical properties, but has a problem of poor workability, particularly wear resistance.
  • the insulated wire is greatly deformed to increase the space factor of the coil. For example, after forming the coil by winding the insulated wire, the coil is inserted into the slot, or the insulated wire deformed in advance is welded to form the coil. If the insulating layer has poor wear resistance, the insulating layer is easily damaged during processing, and the insulating layer may be cracked or pinholed, resulting in poor electrical characteristics.
  • Patent Document 1 a film layer made of polybenzimidazole resin is provided on a polyimide film layer to achieve both heat resistance and wear resistance.
  • the polyimide film is formed by applying and baking a varnish (polyimide resin varnish) obtained by dissolving a polyimide precursor resin in a solvent on a conductor.
  • the polyamic acid which is a polyimide precursor, is imidized by heat during baking to become polyimide. Since only a thin film having a thickness of about several ⁇ m can be formed by a single coating and baking process, a polyimide film having a predetermined thickness (several tens of ⁇ m) is formed by repeating the coating and baking processes a plurality of times.
  • a polyimide resin varnish is applied on the polyimide layer formed in the previous step.
  • the solvent contained in the polyimide resin varnish dissolves the lower layer (polyimide layer formed in the previous step) slightly, so that the compatibility between the layers is improved and the adhesion between the layers is obtained.
  • the baked imidized polyimide is too high in solvent resistance compared to other resins such as polyamideimide, so that the lower layer hardly dissolves when varnish is applied. Accordingly, the adhesion force (adhesive force) between the layers is reduced, and if the processing causes a large deformation in the film, the film is destroyed due to the peeling between the layers.
  • the adhesion between the insulating layer and the conductor is also necessary. If the adhesion between the conductor and the insulating layer is low, floating occurs between the conductor and the insulating layer in the winding process or the process of deforming the insulated wire, and the electrical characteristics deteriorate.
  • the present invention has been made in view of the above problems, and an object thereof is to provide a polyimide resin varnish capable of forming an insulating layer having high interlayer adhesion and adhesion with a conductor and excellent workability. Further, the present invention has an insulating layer formed using the above polyimide resin varnish, an insulated wire that can satisfy required characteristics such as work resistance, heat resistance, mechanical strength, and an electric coil using the same, It is an object to provide a motor.
  • the interlayer adhesion of the polyimide film correlates with the solubility of the polyimide in the solvent.
  • the present inventors paid attention to the imide group concentration of polyimide and found that the solubility in a solvent can be improved by lowering the concentration of a highly polar imide group.
  • a general polyimide resin widely used for a film of an insulated wire is obtained by imidizing a polyimide precursor (polyamic acid) obtained by polymerizing pyromellitic dianhydride and 4,4′-diaminodiphenyl ether.
  • the imide group concentration is 36.6%.
  • the present invention is a polyimide resin varnish mainly composed of a polyimide precursor resin obtained by reacting an aromatic diamine and an aromatic tetracarboxylic dianhydride, It is a polyimide resin varnish whose imide group density
  • concentration after the imidation of the said polyimide precursor resin is 28.0% or more and 33.0% or less (Claim 1).
  • the imide group concentration is (Molecular weight of imide group) / (Molecular weight of all polymers) ⁇ 100 (%) It is a value calculated by. Since the polyimide precursor is obtained by reacting an aromatic diamine and an aromatic tetracarboxylic dianhydride, the imide group concentration is increased when the molecular weight of each monomer (aromatic diamine or aromatic tetracarboxylic dianhydride) increases. Lower.
  • the imide group concentration is lowered, the solubility of the polyimide after imidization is improved and the interlayer adhesion is improved.
  • the highly polar imide group contributes to the adhesion with the conductor, and the adhesion with the conductor decreases when the imide group concentration decreases.
  • the imide group concentration is adjusted by arbitrarily selecting the aromatic diamine and the aromatic tetracarboxylic dianhydride constituting the polyimide precursor so that the imide group concentration is 28.0% or more and 33.0% or less. .
  • the aromatic tetracarboxylic dianhydride is preferably pyromellitic dianhydride (PMDA) (Claim 2).
  • PMDA pyromellitic dianhydride
  • Pyromellitic dianhydride has a relatively small molecular weight and a rigid structure.
  • aromatic diamine or aromatic tetracarboxylic dianhydride has a large molecular weight
  • aromatic tetracarboxylic dianhydride having a large molecular weight is Since heat resistance decreases when used, it is preferable to select PMDA having a low molecular weight and to adjust the imide group concentration using an aromatic diamine having a high molecular weight because the heat resistance is improved.
  • the aromatic diamine comprises 2,2-bis [4- (aminophenoxy) phenyl] propane, 1,3-bis (4-aminophenoxy) benzene, and 1,4-bis (4-aminophenoxy) benzene. It is preferable to contain 1 or more types selected from the group (Claim 3). These aromatic diamines have a large molecular weight and can reduce the imide group concentration. In particular, when PMDA is selected as the aromatic tetracarboxylic dianhydride, the balance between heat resistance and adhesion is preferred. A plurality of aromatic diamines may be used in combination.
  • the imide group concentration by combining the above-described aromatic diamine having a large molecular weight and an aromatic dian having a small molecular weight such as 4,4'-diaminodiphenyl ether (ODA).
  • aromatic diamine having a large molecular weight and an aromatic dian having a small molecular weight such as 4,4'-diaminodiphenyl ether (ODA).
  • ODA 4,4'-diaminodiphenyl ether
  • Invention of Claim 4 is an insulated wire which has a conductor and the insulating layer which coat
  • the invention according to claim 5 is an insulated wire having an insulating layer that directly covers a conductor, and the insulating layer is formed by repeating the steps of applying and baking the polyimide resin varnish a plurality of times. It is an insulated wire. Since the polyimide resin varnish of the present invention is excellent in adhesion and interlaminar adhesion with a conductor, even with an insulated wire having an insulating layer composed of a plurality of layers of polyimide resin in this manner, adhesion with the conductor Workability is improved due to excellent strength and interlayer adhesion. Moreover, since it is possible to form an insulating layer only with the polyimide which is excellent in heat resistance, the heat resistance of an insulated wire can be improved more.
  • the invention according to claim 6 is an electric coil formed by winding the insulated wire.
  • a seventh aspect of the present invention is a motor having the electric coil according to the sixth aspect. Since an insulated wire excellent in workability and heat resistance is used, a coil with a high space factor can be obtained, and the coil and motor can be downsized. Further, even when a high voltage is applied, the insulating film is hardly deteriorated, so that the life can be extended.
  • the present invention it is possible to provide a polyimide resin varnish capable of forming an insulating layer having high interlayer adhesion and adhesion with a conductor and excellent workability. Moreover, the insulated wire of the present invention is excellent in work resistance and can satisfy required characteristics such as heat resistance and mechanical strength.
  • the polyimide precursor resin (polyamic acid) which is the main component of the polyimide resin varnish of the present invention is obtained by condensation polymerization of an aromatic tetracarboxylic dianhydride and an aromatic diamine. This condensation polymerization reaction can be performed under the same conditions as in the conventional synthesis of a polyimide precursor.
  • aromatic tetracarboxylic dianhydrides include pyromellitic dianhydride (PMDA), 4,4′-oxydiphthalic dianhydride (ODPA), 3,4,3 ′, 4′-biphenyltetracarboxylic dianhydride.
  • Anhydride (BPDA), 3,3 ′, 4,4′-benzophenone tetracarboxylic dianhydride (BTDA), 3,3 ′, 4,4′-diphenylsulfone tetracarboxylic dianhydride, bicyclo (2, 2,2) -Oct-7-ene-2,3,5,6-tetracarboxylic dianhydride, 1,2,4,5-cyclohexanetetracarboxylic dianhydride, 2,2-bis (3 4-dicarboxyxyphenyl) hexafluoropropane dianhydride, 5- (2,5-dioxotetrahydrofuryl) -3-methyl-3-cyclohexene-1,2-dicarboxylic dianhydride, etc.
  • pyromellitic dianhydride is preferable because it has a low molecular weight and a rigid structure and can improve the heat resistance of the polyimide resin.
  • Aromatic diamines include 4,4′-diaminodiphenyl ether (ODA), 4,4′-methylenedianiline (MDA), 2,2-bis [4- (aminophenoxy) phenyl] propane (BAPP), 1, 4-bis (4-aminophenoxy) benzene (TPE-Q), 1,3-bis (4-aminophenoxy) benzene (TPE-R), 1,1-bis [4- (4-aminophenoxy) phenyl]
  • Examples include cyclohexane (4-APBZ), 1,3-bis (3-aminophenoxy) benzene (3-APB), 1,5-bis (3-aminophenoxy) naphthalene (1,5-BAPN), and the like.
  • 2,2-bis [4- (aminophenoxy) phenyl] propane (BAPP), 1,3-bis (4-aminophenoxy) benzene (TPE-R), 1,4-bis (4-aminophenoxy) Benzene (TPE-Q) is preferably used because it has a large molecular weight and can reduce the imide group concentration.
  • the imide group concentration can be adjusted by using these aromatic diamines in combination with an aromatic diamine having a small molecular weight such as ODA and MDA.
  • the aromatic tetracarboxylic dianhydride and the aromatic diamine are selected so that the imide group concentration after imidization is 28.0% or more and 33.0% or less.
  • the imide group concentration is (Molecular weight of imide group) / (Molecular weight of all polymers) ⁇ 100 It is a value calculated by. Specifically, the imide group concentration is calculated by the following method.
  • concentration in a unit unit is calculated from the molecular weight of aromatic tetracarboxylic dianhydride and aromatic diamine.
  • aromatic tetracarboxylic dianhydride and aromatic diamine are mixed and reacted.
  • the reaction proceeds favorably, which is preferable.
  • Each material is mixed and heated to react in an organic solvent to obtain a polyimide precursor resin.
  • an aprotic polar organic solvent such as N-methyl-2-pyrrolidone, N, N-dimethylformamide, N, N-dimethylacetamide, dimethyl sulfoxide, ⁇ -butyrolactone can be used. These organic solvents may be used alone or in combination of two or more.
  • the amount of the organic solvent is not particularly limited as long as it is an amount capable of uniformly dispersing the aromatic tetracarboxylic dianhydride and the aromatic diamine, but usually 100 parts by mass per 100 parts by mass of the total amount of these components. Use up to 1000 parts by mass (so that the resin concentration is about 10% to 50%). If the amount of the organic solvent is reduced, the amount of the solid content of the polyimide resin varnish obtained is increased, which is effective for cost reduction.
  • additives such as pigments, dyes, inorganic or organic fillers, lubricants, adhesion improvers, reactive low molecules, compatibilizers, and the like may be added to the polyimide resin varnish.
  • melamine is added as an adhesion improver, adhesion with the conductor can be improved.
  • other resins can be mixed and used within a range not impairing the gist of the present invention.
  • a polyimide resin varnish is applied on a conductor directly or through another layer and baked to form an insulating layer.
  • the polyimide precursor resin is imidized to become polyimide.
  • Application and baking can be performed in the same manner as in the production of a normal insulated wire.
  • an insulating layer is formed by repeating several times of baking in a furnace with a preset temperature of 350 to 500 ° C. for 5 to 10 seconds per pass. The thickness of the insulating layer is 10 ⁇ m to 150 ⁇ m.
  • the conductor copper, copper alloy, aluminum, or the like can be used.
  • the size of the conductor and the cross-sectional shape thereof are not particularly limited, but in the case of a round wire, a conductor diameter of 100 ⁇ m to 5 mm is generally used, and in the case of a flat wire, one having a side length of 500 ⁇ m to 5 mm is generally used.
  • the insulating layer may be a single layer or multiple layers.
  • the insulating layer is a single layer, only the insulating layer formed by applying and baking the above polyimide resin varnish becomes the insulating layer.
  • the insulating layer has a multilayer structure, another insulating layer is formed before or after the formation of the insulating layer made of polyimide.
  • the resin for forming the other insulating layer any resin such as polyimide, polyamideimide, polyesterimide, polyurethane, and polyetherimide can be used.
  • the outermost layer has a surface lubricating layer as the insulating layer because the workability is further improved. Moreover, you may apply
  • FIG. 1 is a schematic sectional view showing an example of an insulated wire of the present invention.
  • a multi-layer insulating layer is provided outside the conductor 3, and the insulating layers are a first insulating layer 1 and a second insulating layer 2 from the conductor side.
  • the first insulating layer 1 and the second insulating layer 2 are all formed by applying and baking the polyamide-imide resin varnish of the present invention, an insulated wire having excellent heat resistance and excellent adhesion to conductors and interlayer adhesion is obtained. can get. Further, in order to further improve the adhesion with the conductor, other resins such as polyamideimide may be used as the first insulating layer 1.
  • the insulated wire of the present invention is not limited to this shape.
  • FIG. 2 (a) is a schematic view showing an example of the electric coil of the present invention
  • FIG. 2 (b) is a cross-sectional view taken along the line A-A 'of FIG. 2 (a).
  • the electric wire 12 is formed by winding the insulated wire 11 outside the core 13 made of a magnetic material.
  • a member composed of a core and an electric coil is used as a rotor or a stator of a motor.
  • a stator 15 in which a plurality of divided stators 14 each composed of a core 13 and an electric coil 12 are combined and arranged in an annular shape is used as a constituent member of a motor.
  • An insulating layer having a thickness of about 40 ⁇ m was formed on the surface of a flat conductor having a thickness of 1.5 mm and a width of 3.0 mm by repeating the steps of applying and baking the produced polyimide resin varnish by a conventional method several times. Insulated wires of Comparative Examples 1 to 5 were produced.
  • Examples 1 to 3 and Comparative Examples 1 to 3 ODA having a low molecular weight and BAPP having a high molecular weight are used in combination as an aromatic diamine, and the ratio of BAPP (modified amount of long-chain diamine in the table) is 0% to 100%.
  • the imide group concentration was adjusted by changing. The higher the BAPP ratio and the lower the imide group concentration, the higher the interlayer adhesion. Further, the conductor adhesion is lower as the imide group concentration is lower.
  • the imide group concentration is 28.0% or more and 33.0% or less
  • both the conductor adhesion strength and the interlayer adhesion strength are 50 g / mm or more, and it is estimated that the workability is good.

Abstract

L'invention concerne un vernis de résine de polyimide apte à former une couche isolante ayant une adhérence inter-couches élevée, une adhérence élevée à un conducteur et une excellente résistance de traitement. L'invention concerne également un fil électrique isolé ayant une excellente résistance de traitement, une excellente résistance à la chaleur et d'excellentes propriétés mécaniques. Le vernis de résine de polyimide a comme composant principal de celui-ci une résine précurseur de polyimide obtenue par réaction d'une diamine aromatique et d'un dianhydride tétracarboxylique aromatique. La concentration en groupe imide de la résine précurseur de polyimide après imidation est de 28,0 %-33,0 %.
PCT/JP2012/061047 2011-05-09 2012-04-25 Vernis de résine de polyimide, fil électrique isolé l'utilisant, bobine électrique et moteur WO2012153636A1 (fr)

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JP2011103948A JP2012233123A (ja) 2011-05-09 2011-05-09 ポリイミド樹脂ワニス及びそれを用いた絶縁電線、電機コイル、モータ
JP2011-103948 2011-05-09

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JP6012672B2 (ja) * 2014-07-14 2016-10-25 古河電気工業株式会社 絶縁被覆アルミニウム電線
JP6614953B2 (ja) 2015-12-08 2019-12-04 古河電気工業株式会社 絶縁電線、コイルおよび電気・電子機器
CN109054018B (zh) * 2018-06-06 2021-05-14 华南理工大学 一种聚酰胺酸溶液及其制备方法
CN108794748B (zh) * 2018-06-06 2021-08-10 华南理工大学 一种低介电常数的聚酰亚胺薄膜及其制备方法
CN112020532B (zh) 2019-03-29 2023-07-28 埃赛克斯古河电磁线日本有限公司 绝缘电线、线圈、以及电气/电子设备

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Publication number Priority date Publication date Assignee Title
JPS63221126A (ja) * 1987-03-09 1988-09-14 Kanegafuchi Chem Ind Co Ltd 吸水特性に優れたポリイミド樹脂
JP2001266647A (ja) * 2000-03-23 2001-09-28 Unitika Ltd 絶縁被覆物及びそれを得るための絶縁塗料
JP2003119380A (ja) * 2001-10-05 2003-04-23 Du Pont Toray Co Ltd 難燃性成形体、照明機器用反射体基材および照明機器用反射体
WO2007083526A1 (fr) * 2006-01-20 2007-07-26 Kaneka Corporation Film polyimide et utilisation correspondante

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS63221126A (ja) * 1987-03-09 1988-09-14 Kanegafuchi Chem Ind Co Ltd 吸水特性に優れたポリイミド樹脂
JP2001266647A (ja) * 2000-03-23 2001-09-28 Unitika Ltd 絶縁被覆物及びそれを得るための絶縁塗料
JP2003119380A (ja) * 2001-10-05 2003-04-23 Du Pont Toray Co Ltd 難燃性成形体、照明機器用反射体基材および照明機器用反射体
WO2007083526A1 (fr) * 2006-01-20 2007-07-26 Kaneka Corporation Film polyimide et utilisation correspondante

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