EP2533251B1 - Electrical insulating material and high voltage equipment - Google Patents

Electrical insulating material and high voltage equipment Download PDF

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Publication number
EP2533251B1
EP2533251B1 EP20120156022 EP12156022A EP2533251B1 EP 2533251 B1 EP2533251 B1 EP 2533251B1 EP 20120156022 EP20120156022 EP 20120156022 EP 12156022 A EP12156022 A EP 12156022A EP 2533251 B1 EP2533251 B1 EP 2533251B1
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EP
European Patent Office
Prior art keywords
insulating material
electrical insulating
rubber
particle
resin
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Legal status (The legal status 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 status listed.)
Not-in-force
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EP20120156022
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German (de)
English (en)
French (fr)
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EP2533251A1 (en
Inventor
Hironori Matsumoto
Atsushi Ootake
Masaki Takeuchi
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Hitachi Industrial Equipment Systems Co Ltd
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Hitachi Industrial Equipment Systems Co Ltd
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    • 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

Definitions

  • the present invention relates to an electrical insulating material and a high voltage equipment in which the insulating material is applied at a site requiring an electrical insulation.
  • a gaseous insulation with an insulating gas, a vacuum insulation, or an oil insulation, in which an insulating oil is encapsulated has been a conventional mainstream of an insulation system which is applied to a transmission and distribution equipment including a transformer and a circuit breaker, or to a high voltage equipment such as a motor and an inverter.
  • a solid insulation system in which a solid insulation material having a good insulation strength is adopted, is advanced.
  • thermosetting resin such as an epoxy resin is in heavy usage due to its excellent insulation properties, heat resisting properties, mechanical characteristics, and chemical stability.
  • thermosetting resin is large in a thermal expansion coefficient as compared with metals, its surface in contact with a dissimilar material becomes very high in a thermal stress due to a differential thermal expansion.
  • an inorganic particle having a very small thermal expansion coefficient such as silica or alumina, is added to the resin in a large amount.
  • an excessive addition of the inorganic particle considerably increases the viscosity of the resin to reduce a workability. Further, it may cause a void in the resin hardened material.
  • the void in the resin hardened material is in danger of causing a decrease in insulation properties due to a concentration of an electric field, or a decrease in a mechanical strength. Accordingly, the technology of highly filling an inorganic particle, the technology of making the low viscosity of the resin, or the technology of making the high strength, whereby crack resistance properties are provided to the resin itself to inhibit a crack in the resin, has been eagerly considered.
  • Patent Document 1 discloses a method wherein an ultrafine particle thermoplastic resin, epoxy resin, a curing agent, an inorganic filler, and a hardening accelerator are mixed with each other whereby a resin excellent in adhesive property and toughness is provided.
  • Patent Document 2 discloses a method in which to a thermosetting resin comprising an epoxy resin and a curing agent, an inorganic particle having different ⁇ m sizes and a rubber particle comprising a core-shell structure are added whereby an electrical insulating material excellent in mechanical properties is provided.
  • Patent Document 1 does not refer to a method of manufacturing the ultrafine particle thermoplastic resin.
  • a thermoplastic resin is commonly and preliminarily cross-linked to be formed and shaped to a finite size.
  • an impurity such as sulfur is apt to be incorporated due to the use of a vulcanizing agent as a cross-linking agent.
  • an insulating material including such an impurity is arranged in close vicinity to a conducting body, the progression of a migration, which is caused due to a moisture absorption or the like, may be accelerated to remarkably lower insulation performance.
  • Patent Document 2 selects a core-shell type of rubber particles as elastomer particles.
  • the core-shell type comprises a structure having a core layer having the elastomer particles within the rubber particle, and a further shell layer which is compatible with the resin and provided at the outer side, whereby the dispersibility of the elastomer particles in the resin is enhanced and the crack resistance properties of the resin can be stably enhanced.
  • the core-shell type of elastomer particles are used, according to our experiments it has been confirmed that the effects can not be derived without an addition in a large amount.
  • An object of the present invention is to provide an electrical insulating material excellent in crack resistance properties without deteriorating the properties of an insulating resin in a solid insulation system, and a high voltage equipment using the same.
  • the present invention provides an electrical insulating material comprising:
  • the present invention can obtain an electrical insulating material excellent in crack resistance properties without deteriorating its properties (a thermal resistance and insulation properties), and a high voltage equipment to which the electrical insulating material is applied.
  • the epoxy resin in the present invention is a compound including two or more epoxy groups comprising two carbon atoms and one oxygen atom within its molecule, while the epoxy group can be subjected to a ring-opening reaction with an appropriate curing agent, and as the epoxy resin, any one can be applied, provided that it can be formed into a hardened resin material.
  • a bisphenol A type epoxy resin which can be derived by the condensation of epichlorohydrin with a polyhydric phenol or polyhydric alcohol such as bisphenols
  • a bisphenol A type epoxy resin which can be derived by the condensation of epichlorohydrin with a polyhydric phenol or polyhydric alcohol such as bisphenols
  • a brominated bisphenol A type epoxy resin a hydrogenated bisphenol A type epoxy resin
  • a bisphenol F type epoxy resin a bisphenol S type epoxy resin
  • a bisphenol AF type epoxy resin a biphenyl type epoxy resin; a naphthalene type epoxy resin; a fluorene type epoxy resin; a novolac type epoxy resin; a phenolnovolac type epoxy resin; an ortho-cresol novolac type epoxy resin; a tris(hydroxyphenyl)methane type epoxy resin; a glycidyl ether type of epoxy resin such as tetraphenylolethane type epoxy resins
  • an elastomer particle derived by a radiation cross-linking is excellent in a thermal resistance due to its high crosslink density, and further a difference in crosslink density between the elastomer particles is small due to a homogeneous progress in cross-linking so that crack resistance properties can be stably enhanced. Furthermore, since the radiation cross-linking is progressed merely by irradiating radiation rays (electron beams), it is not necessary to add an extra cross linking agent, and thus for example, impurities such as sulfur in a vulcanizing agent used as a cross linking agent are difficult to incorporate. As a result, a migration, whose progress is accelerated with an impurity element, can be inhibited.
  • the radiation cross-linked elastomer particle when according to the present invention the radiation cross-linked elastomer particle is used, the crack resistance properties of the resin is undoubtedly enhanced, the resin has excellent insulation properties including the inhibition of migration, and further the decrease of a thermal resistance can be inhibited.
  • the presence or absence of the radiation cross-linked elastomer particle can be evaluated through a chemical analysis such as a solid NMR.
  • the average particle size of elastomer particles is preferably 500 nm or less, and more preferably 100 nm or less, and the elastomer particle is preferably uniformly dispersed in an electrical insulating material.
  • Table 1 shows a relationship among a spheric particle radius, an interparticle distance, and a relative specific surface area in a disperse system having a volume concentration of 2%.
  • Table 1 Table 1 Particle radius [nm] Interparticle distance [nm] Particle specific surface area 40000 160000 1 4000 1600 100 4 16 10000
  • an amount of the elastomer particle added is preferably 50 parts by weight or less relative to 100 parts by weight of the epoxy resin, and more preferably 30 parts by weight or less.
  • the amount of the elastomer particle added is more preferably 30 parts by weight or less relative to 100 parts by weight of the epoxy resin.
  • a part (or the whole) of the elastomer particle preferably comprises any one of acrylic rubber, nitrile rubber, isoprene rubber, urethane rubber, ethylene propylene rubber, epichlorohydrin rubber, chloroprene rubber, styrene rubber, silicone rubber, fluoro rubber or butyl rubber, or a modified material thereof, or a combination thereof, and a surface or inside thereof is modified with any one of a carboxyl group, acid anhydrides, amines or imidazoles, or a combination thereof.
  • the rubbers mentioned above are ones which are industrially produced, and are inexpensively available.
  • the elastomer particle in order to enhance a compatibility between the elastomer particle and the resin, can be modified with any one of a carboxyl group, acid anhydrides, amines and imidazoles, a combination thereof, whereby the elastomer particle can be uniformly and easily dispersed in the resin.
  • the elastomer particle can be preliminarily dispersed in the epoxy resin and a curing agent, whereby the compatibility between the elastomer particle and the resin can be enhanced.
  • a part of the elastomer particle preferably comprises the elastomer particle mentioned above, and an elastomer particle except the above part of the elastomer particle preferably comprises a core-shell type of an elastomer particle.
  • Radiation cross-linked elastomer particle according to the present invention preferably has an average particle size of 100 nm or less, while in a system wherein the elastomer particle is mixed with a core-shell type of elastomer particle, the average particle size of the core-shell type of elastomer particle is preferably in the range of approximately from 100 nm to several hundreds nm for the purpose of suppressing a remarkable increase in material cost, such an elastomer particle being commercially available.
  • the amount of a core-shell type of elastomer particle added in a conventional resin can be decreased, and a decrease in resin properties such as insulation properties, and a thermal resistance can be inhibited to a minimum, while crack resistance properties can be more stably obtained.
  • a part or the whole of the inorganic particle is preferably any one of silica (SiO 2 ), alumina (Al 2 O 3 ), alumina hydrate, titanium oxide (TiO 2 ), aluminum nitride (AlN) or boron nitride (BN), or a combination thereof, and preferably has an average particle size of 500 ⁇ m or less.
  • the addition of the inorganic particle can decrease the thermal expansion of the resin to inhibit the occurrence of resin peeling or resin crack at a site wherein the resin is in contact with a dissimilar material.
  • silica of inorganic materials corresponding to this, a natural silica (a crushed silica), a molten silica, and a crystal silica can be enumerated, while as alumina, for example, a low-soda alumina, and an easily sinterable alumina can be enumerated.
  • Aluminum nitride and boron nitride are high cost, but excellent in thermal conductivity performance, and thus are preferred for the purpose of enhancing the thermal conductivity of a hardened material.
  • these inorganic particle has an average particle size of 500 ⁇ m or less, and a wide particle size distribution in the range of from 0.1 ⁇ m to 100 ⁇ m. Thereby, even when inorganic particles are highly filled, making a low viscosity is feasible.
  • a surface of the inorganic particle is preferably modified with any one selected from the group consisting of a group comprising a hydrocarbon, such as an alkyl group, an acrylic group, a methacrylic group, a hydroxyl group, acid anhydrides, imidazoles, amines, a carboxyl group, and an alkoxyl group, or a combination thereof.
  • a hydrocarbon such as an alkyl group, an acrylic group, a methacrylic group, a hydroxyl group, acid anhydrides, imidazoles, amines, a carboxyl group, and an alkoxyl group, or a combination thereof.
  • an amount of the inorganic particle added is preferably from 300 to 600 parts by weight relative to 100 parts by weight of the epoxy resin.
  • the amount of the inorganic particle is more than 300 parts by weight, the thermal expansion coefficient of the resin is remarkably large, so that the peeling or resin crack at a joint area is easily caused. Further, when more than 600 parts by weight, the resin viscosity is remarkably increased, whereby the workability is lowered, while defects are caused in the hardened material, so that mechanical properties and electrical properties are lowered.
  • the curing agent preferably comprises acid anhydrides.
  • Other curing agents for the epoxy resin can include amines, imidasoles, phenol resins, hydrazides in addition to acid anhydrides, while an epoxy resin using an acid anhydride curing agent has a long usable time, and further electrical, chemical and mechanical properties can be provided in a balanced manner.
  • the acid anhydride curing agent can include, for example, dodecenylsuccinic anhydride, poly(adipic anhydride), poly(azelaic anhydride), poly(sebacic anhydride), poly(ethyloctadecanedioic anhydride), poly(phenylhexadecanedioic anhydride), methyltetrahydrophthalic anhydride, methylhexahydrophthalic anhydride, methyl himic anhydride, hexahydrophthalic anhydride, tetrahydrophthalic anhydride, trialkyltetrahydrophthalic anhydride, methylcyclohexene dicarboxylic anhydride, phthalic anhydride, trimellitic anhydride, pyromellitic dianhydride, benzophenone tetracarboxylic acid, ethylene glycol bistrimellitate, glycerol tristrimellitate, chlorendic anhydride, te
  • a hardening accelerator for epoxy compounds which promotes or controls the curing reaction of the epoxy compound can be used at the same time.
  • the curing reaction is slow as compared to the one of other curing agent such as an amine system curing agent, and thus the hardening accelerator for epoxy compounds can be often applied.
  • the hardening accelerator for epoxy compounds can include a tertiary amine and a salt thereof, a quaternary ammonium compound, imidazole, alkali metal alkoxide, and the like.
  • a silane coupling agent, a titanate coupling agent, or other surface modifying agent for the inorganic particle and elastomer particle can be further added.
  • the silane coupling agent enhances wetting properties between the resin and the inorganic particle, while strengthens an adhesion between the resin and the inorganic particle.
  • the tinanate coupling agent makes a low viscosity and enhances the mechanical properties of the hardened material.
  • a device for mixing is not limited, provided that the device can mix a liquid to be treated, strongly providing to the liquid a shearing force and/or a load for stretching.
  • a rotary and revolutionary type of mixer, a homogenizer, a dissolver type of mixer, a homomixer, a ball mill, or a triple roll mill can be used.
  • a viscosity of the electrical insulating material manufactured according to the present invention is preferably 150 Pa ⁇ s or less at 80°C, and more preferably 20 Pa ⁇ s or less.
  • the electrical insulating material is chiefly inpoured into a vessel such as a die, within which a site requiring an electrical insulation is disposed, to be cast into a predetermined shape. Therefore, when the resin viscosity is more than 150 Pa ⁇ s, voids are caused without the resin being inpoured in every detail to lower mechanical and/or electrical properties. Further, for the purpose of the decrease of resin viscosity, the resin, a die, a working bench, and the like are previously and preliminarily heated to approximately 80°C. On this occasion, when the resin viscosity is 20 Pa ⁇ s or less, the resin can be inpoured into a vessel such as a die, and resultantly the mechanical and/or electrical properties of the hardened material can be stably obtained.
  • the present invention further provides a high voltage equipment, in which said electrical insulating material according to claim 1 is applied at a site requiring an electrical insulation of an electrical equipment.
  • the electrical insulating material mentioned above can be applied to the high voltage equipment such as a transformer, a circuit breaker, a motor, or an inverter.
  • Table 2 shows the compounding composition of epoxy resins, inorganic particles, and elastomer particles in each of Examples 1 to 3, and Comparative Examples 1 to 3.
  • Figure 2 shows a sectional view wherein an electrical insulating material according to the present invention is applied to a transformer.
  • Tables 3 and 4 show the results of the properties evaluation of resins in Examples and Comparative Examples.
  • epoxy resins bisphenol A type and bisphenol F type
  • 10 parts by weight of a radiation cross-linked acrylonitrile-butadiene rubber particles (having an average particle size of 50 to 100 nm) modified with carboxylic acid 415 parts by weight of crushed silica as inorganic particles were added.
  • an anhydride curing agent, a silane coupling agent, a titanate coupling agent, and an imidazole compound as a hardening accelerator were suitably added thereto, followed by kneading the same with the addition of a sufficient shearing force in a state of heating at 80°C. After defoaming the prepared mixed liquid, the same was cured under a heating condition of 100°C/5 hours plus 170°C/7 hours to prepare a hardened material.
  • epoxy resins bisphenol A type and bisphenol F type
  • 10 parts by weight of a radiation cross-linked acrylonitrile-butadiene rubber particles (having an average particle size of 50 to 100 nm) modified with carboxylic acid 300 parts by weight of crushed silica as inorganic particles were added.
  • an anhydride curing agent, a silane coupling agent, a titanate coupling agent, and an imidazole compound as a hardening accelerator were suitably added thereto, followed by kneading the same with the addition of a sufficient shearing force in a state of heating at 80°C. After defoaming the prepared mixed liquid, the same was cured under a heating condition of 100°C/5 hours plus 170°C/7 hours to prepare a hardened material.
  • epoxy resins bisphenol A type and bisphenol F type
  • 8 parts by weight of a radiation cross-linked acrylonitrile-butadiene rubber particles (having an average particle size of 50 to 100 nm) modified with carboxylic acid 600 parts by weight of crushed silica as inorganic particles were added.
  • an anhydride curing agent, a silane coupling agent, a titanate coupling agent, and an imidazole compound as a hardening accelerator were suitably added thereto, followed by kneading the same with the addition of a sufficient shearing force in a state of heating at 80°C. After defoaming the prepared mixed liquid, the same was cured under a heating condition of 100°C/5 hours plus 170°C/7 hours to prepare a hardened material.
  • An electrical insulating material according to the present invention was applied to a transformer. As shown in Fig. 2 , a primary winding, a secondary winding, an interlayer isolation material, an iron core, and constituent elements thereof were molded with the electrical insulating material. In the same structure, temperature change in operation, or temperature change in transit locally causes thermal stress in the electrical insulating material, the occurrence of crack and resins breaking are inhibited due to having crack resistance properties. Furthermore, due to high thermal resistance, the resin properties at a high temperature are also excellent, and in addition to crack resistance properties, the decrease of other mechanical properties is inhibited.
  • an electrical insulating material according to the present invention is low in viscosity, even in the vicinity of a winding wire or an interlayer insulator, it can be filled with no space therebetween. As a result, insulation properties and mechanical strength become high. Accordingly, it can be applied even to a small transformer being large in thermal and electrical stress.
  • epoxy resins bisphenol A type and bisphenol F type
  • 415 parts by weight of crushed silica as inorganic particles were added.
  • an anhydride curing agent, a silane coupling agent, a titanate coupling agent, and an imidazole compound as a hardening accelerator were suitably added thereto, followed by kneading the same with the addition of a sufficient shearing force in a state of heating at 80°C. After defoaming the prepared mixed liquid, the same was cured under a heating condition of 100°C/5 hours plus 170°C/7 hours to prepare a hardened material.
  • epoxy resins bisphenol A type and bisphenol F type
  • 300 parts by weight of crushed silica as inorganic particles were added.
  • an anhydride curing agent, a silane coupling agent, a titanate coupling agent, and an imidazole compound as a hardening accelerator were suitably added thereto, followed by kneading the same with the addition of a sufficient shearing force in a state of heating at 80°C.
  • the same was cured under a heating condition of 100°C/5 hours plus 170°C/7 hours to prepare a hardened material.
  • epoxy resins bisphenol A type and bisphenol F type
  • 8 parts by weight of a core-shell type of fine rubber particle having an average particle size of 100 to 500 nm
  • its core layer comprises butadiene rubber
  • 600 parts by weight of crushed silica as inorganic particles were added.
  • an anhydride curing agent, a silane coupling agent, a titanate coupling agent, and an imidazole compound as a hardening accelerator were suitably added thereto, followed by kneading the same with the addition of a sufficient shearing force in a state of heating at 80°C. After defoaming the prepared mixed liquid, the same was cured under a heating condition of 100°C/5 hours plus 170°C/7 hours to prepare a hardened material.
  • each of fracture toughness, coefficient of linear expansion, and deformation temperature was determined in the following manner.
  • the coefficient of linear expansion of the hardened material was determined using a thermomechanical analysis apparatus (TMA).
  • TMA thermomechanical analysis apparatus
  • the rate of temperature rise was set to be 5°C/minute.
  • the hardened material was preheated to 160°C, and thereafter slowly cooled, followed by determination.
  • the deformation temperature of a hardened material was determined using TMA in a similar manner.
  • the rate of temperature rise was set to be 5°C/min. Further, in order to remove the distortion of the hardened material, the hardened material was preheated to 160°C, and thereafter slowly cooled, followed by determination.
  • Comparative results of fracture toughness according to Example 1 and Comparative Example 1 are shown in Table 3, while comparative results of fracture toughness, coefficient of linear expansion, and deformation temperature according to Example 2 and Comparative Example 2 are shown in Table 4. Besides, comparative results of fracture toughness according to Example 3 and Comparative Example 3 are shown in Table 5. Incidentally, the values in each Table were put into shape by being normalized based on the value of each Comparative Example. With reference to these results, the specific advantageous effects of the present invention will be explained hereinafter.
  • Example 3 can explain the advantageous effect that fracture toughness is enhanced by mixing finer elastomer particles and the resin, that is, crack resistance properties are enhanced.
  • Example 3 according to the present invention enhanced fracture toughness, that is, enhanced crack resistance properties as compared to Comparative Example 3 wherein coarser elastomer particles were used. This is an advantageous effect derived from the fact that an interacting region between the particles and the resin has been spread out by the use of the finer elastomer particles, and the enhancement effect of fracture toughness has been increased as compared with a case wherein coarser elastomer particles were used.

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  • Physics & Mathematics (AREA)
  • Spectroscopy & Molecular Physics (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Organic Insulating Materials (AREA)
  • Inorganic Insulating Materials (AREA)
EP20120156022 2011-06-10 2012-02-17 Electrical insulating material and high voltage equipment Not-in-force EP2533251B1 (en)

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JP2011129747A JP5587248B2 (ja) 2011-06-10 2011-06-10 電気絶縁材料およびこれを用いた高電圧機器

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EP2533251A1 EP2533251A1 (en) 2012-12-12
EP2533251B1 true EP2533251B1 (en) 2014-08-06

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JP (1) JP5587248B2 (ja)
CN (1) CN102816411B (ja)
IN (1) IN2012DE00444A (ja)

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JP2014129466A (ja) * 2012-12-28 2014-07-10 Hitachi Industrial Equipment Systems Co Ltd 高電圧機器用絶縁樹脂材およびそれを用いた高電圧機器
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CN103951935B (zh) * 2014-03-10 2016-04-06 哈尔滨理工大学 SiO2-Al2O3/PU-EP复合材料及制备方法
CN103897345B (zh) * 2014-03-10 2016-04-06 哈尔滨理工大学 TiO2/PU-EP复合材料的制备方法
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JPWO2017098566A1 (ja) * 2015-12-07 2018-08-30 株式会社日立製作所 高電圧機器用電気絶縁材料
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JP2018150446A (ja) * 2017-03-13 2018-09-27 株式会社日立製作所 電気絶縁樹脂材料
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IN2012DE00444A (ja) 2015-06-05
JP5587248B2 (ja) 2014-09-10
CN102816411A (zh) 2012-12-12
JP2012255116A (ja) 2012-12-27
EP2533251A1 (en) 2012-12-12
CN102816411B (zh) 2015-11-18

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