JP6458350B2 - Manufacturing method of prepreg tape - Google Patents
Manufacturing method of prepreg tape Download PDFInfo
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- JP6458350B2 JP6458350B2 JP2014081026A JP2014081026A JP6458350B2 JP 6458350 B2 JP6458350 B2 JP 6458350B2 JP 2014081026 A JP2014081026 A JP 2014081026A JP 2014081026 A JP2014081026 A JP 2014081026A JP 6458350 B2 JP6458350 B2 JP 6458350B2
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Description
本発明は、プリプレグテープの製造方法に関する。 The present invention relates to a method for producing a prepreg tape.
電機子巻線の周囲を絶縁層で覆い、水素ガス又は空気を通して冷却する間接冷却方式の発電機において、絶縁層の厚み方向に対する高熱伝導化が望まれている。 In an indirect cooling generator in which an armature winding is covered with an insulating layer and cooled through hydrogen gas or air, it is desired to increase the thermal conductivity in the thickness direction of the insulating layer.
電機子巻線の絶縁層には、樹脂と裏打ち材とマイカからなるプリプレグテープがよく使用される。前記プリプレグテープの高熱伝導化には、多くの場合、テープ中に樹脂及びマイカよりも熱伝導率の高い無機充填粒子を加える方法が提案されている。 A prepreg tape made of a resin, a backing material and mica is often used for the insulating layer of the armature winding. In order to increase the thermal conductivity of the prepreg tape, in many cases, a method of adding inorganic filler particles having higher thermal conductivity than resin and mica to the tape has been proposed.
特許文献１には、無機充填粒子として熱伝導率の高い窒化ホウ素を加えたプリプレグテープが提案されており、０．４０Ｗ／（ｍ・Ｋ）の熱伝導率が得られるとされる。
特許文献２には、マイカ中に熱伝導率の高いアルミナを加えたプリプレグテープの製造方法が提案されており、０．３２〜０．３６Ｗ／（ｍ・Ｋ）の熱伝導率が得られるとされる。
無機充填材を添加していない従来品のプリプレグテープの熱伝導率は０．３０Ｗ／（ｍ・Ｋ）程度であることが知られている。
実用性の観点から、従来品に比較して２倍以上の熱伝導率が得られることが好ましいが、従来品の２倍以上の熱伝導率を得るためには、窒化ホウ素の含有量をマイカを除く全固形分に対して２５体積％〜３５体積％とすることが好ましい。
樹脂に２５体積％〜３５体積％の窒化ホウ素を加え、ロールコーターで塗工可能な無機充填材入り樹脂とするためには、有機溶剤を５質量％以上、４０質量％以下加える必要がある。
It is known that the thermal conductivity of a conventional prepreg tape to which no inorganic filler is added is about 0.30 W / (m · K) .
From the standpoint of practicality, it is preferable to obtain a thermal conductivity that is at least twice that of the conventional product, but in order to obtain a thermal conductivity that is at least twice that of the conventional product, the boron nitride content must be reduced to mica. It is preferable to set it as 25 volume%-35 volume% with respect to the total solid content except this.
In order to add 25% by volume to 35% by volume of boron nitride to the resin to obtain a resin with an inorganic filler that can be applied by a roll coater, it is necessary to add 5% by mass or more and 40% by mass or less of an organic solvent.
有機溶剤としてメチルエチルケトンを５質量％以上、４０質量％以下加えたプリプレグテープを１１０℃で１０分、さらに１７０℃で６０分硬化させた際の動的粘弾性試験から得られたガラス転移温度は１４０℃〜１６０℃である。無機充填材を添加していない従来品のプリプレグテープを同様に硬化させ動的粘弾性試験から得たガラス転移温度は１８０℃であり、耐熱性の観点から、上記有機溶剤量を加えることは好ましくない。 The glass transition temperature obtained from a dynamic viscoelasticity test when a prepreg tape to which methyl ethyl ketone is added as an organic solvent in an amount of 5% by mass to 40% by mass is cured at 110 ° C. for 10 minutes and further at 170 ° C. for 60 minutes is 140. ° C to 160 ° C. A glass transition temperature obtained from a dynamic viscoelasticity test by similarly curing a conventional prepreg tape not containing an inorganic filler is 180 ° C. From the viewpoint of heat resistance, it is preferable to add the amount of the organic solvent. Absent.
さらに、有機溶剤としてメチルエチルケトンを５質量％以上、４０質量％以下加えた無機充填材入り樹脂を塗工したプリプレグテープは、樹脂が塗工されている部分と塗工されていない部分が縦筋状に現れ、外観が悪く、絶縁耐電圧が低下することがある。 Furthermore, the prepreg tape coated with a resin containing an inorganic filler containing 5% by mass or more and 40% by mass or less of methyl ethyl ketone as an organic solvent has a vertical stripe shape where the resin is coated and the uncoated part. Appearing, the appearance is poor, and the dielectric strength voltage may be reduced.
本発明は、高熱伝導率及び高耐熱性を有し、シート外観の良好なプリプレグテープの製造方法を提供することを目的とする。 An object of this invention is to provide the manufacturing method of a prepreg tape which has high heat conductivity, high heat resistance, and favorable sheet | seat external appearance.
前記課題を解決するための具体的手段は以下の通りである。 Specific means for solving the above problems are as follows.
＜１＞ 無機鱗片状粒子を水に混合し濾過乾燥することで無機鱗片状粒子ペーパーを得る第１の工程と、熱硬化性樹脂及び硬化促進剤と、無機充填材と、有機溶剤１質量％〜４質量％あるいは有機溶剤と反応希釈剤の混合液１質量％〜２０質量％とを含む無機充填材入り樹脂を得る第２の工程と、前記第１の工程で得られた無機鱗片状粒子ペーパーと裏打ち材を前記第２の工程で得られた無機充填材入り樹脂を介して貼り合せる第３の工程と、からなるプリプレグテープの製造方法。 <1> First step of obtaining inorganic scaly particle paper by mixing inorganic scaly particles in water and filtering and drying, a thermosetting resin and a curing accelerator, an inorganic filler, and 1% by mass of an organic solvent A second step of obtaining a resin containing an inorganic filler containing 4% by mass or 1% by mass to 20% by mass of a mixed solution of an organic solvent and a reaction diluent, and the inorganic scaly particles obtained in the first step And a third step in which the paper and the backing material are bonded together via the inorganic filler-containing resin obtained in the second step.
＜２＞ 前記無機鱗片状粒子としてマイカを含み、前記マイカをＪＩＳ標準篩を用いて篩い分けした時の粒子径が２．８ｍｍ以上のマイカ片が５０質量％以上である＜１＞に記載のプリプレグテープの製造方法。 <2> As described in <1>, mica is included as the inorganic scaly particles, and a mica piece having a particle diameter of 2.8 mm or more when sieving the mica using a JIS standard sieve is 50% by mass or more. Manufacturing method of prepreg tape.
＜３＞ 前記無機充填材として平均粒子径が１μｍ以上４０μｍ以下である窒化ホウ素を５質量％〜２４質量％含む＜１＞又は＜２＞に記載のプリプレグテープの製造方法。 <3> The method for producing a prepreg tape according to <1> or <2>, wherein the inorganic filler contains 5% by mass to 24% by mass of boron nitride having an average particle diameter of 1 μm or more and 40 μm or less.
本発明によれば、高熱伝導率及び高耐熱性を有し、シート外観の良好なプリプレグテープの製造方法を提供することができる According to the present invention, it is possible to provide a method for producing a prepreg tape having high thermal conductivity and high heat resistance and good sheet appearance.
図１は、本発明のプリプレグテープの製造方法により製造されたプリプレグテープ部材の断面図を示している。このプリプレグテープ部材は、無機鱗片状粒子４を含む層と、裏打ち材２と無機充填材入り樹脂を含む層からなる。前記無機充填材入り樹脂は、無機充填材１、熱硬化性樹脂３、硬化促進剤、及び有機溶剤１質量％〜４質量％あるいは有機溶剤と反応希釈剤の混合液１質量％〜２０質量％を含む。
FIG. 1 shows a cross-sectional view of a prepreg tape member produced by the prepreg tape production method of the present invention. This prepreg tape member is composed of a layer containing
ここで、無機鱗片状粒子としては、マイカであり、ＪＩＳ標準篩を用いて篩い分けした時の粒子径が２．８ｍｍ以上のマイカ片が５０質量％以上であることが好ましい。 Here, the inorganic scaly particles are mica, and the mica pieces having a particle diameter of 2.8 mm or more when sieved using a JIS standard sieve are preferably 50% by mass or more.
裏打ち材としては、例えば、高分子材料で構成される繊維を全部又は一部用いて得られるクロスを用いてもよい。クロスを構成する高分子材料としてはアラミド、ポリイミド、ポリエステル等が挙げられる。高分子材料を繊維の一部として用いる場合には、クロスの縦糸、あるいは横糸又はその両方として用いてもよい。ガラス繊維で構成されるガラスクロスと高分子フィルムを併用してもよい。 As the backing material, for example, a cloth obtained by using all or a part of fibers made of a polymer material may be used. Examples of the polymer material constituting the cloth include aramid, polyimide, polyester, and the like. When the polymer material is used as a part of the fiber, it may be used as a warp yarn, a weft yarn, or both. A glass cloth composed of glass fibers and a polymer film may be used in combination.
無機充填材としては、窒化ホウ素を用いることができ、六方晶窒化ホウ素（ｈ−ＢＮ）、立方晶窒化ホウ素（ｃ−ＢＮ）、ウルツ鉱型窒化ホウ素等が挙げられる。これらの中でも、特に六方晶窒化ホウ素（ｈ−ＢＮ）が好ましい。窒化ホウ素は、鱗片状の一次粒子であってもよく、一次粒子が凝集されて形成される二次粒子であってもよい。 As the inorganic filler, boron nitride can be used, and examples thereof include hexagonal boron nitride (h-BN), cubic boron nitride (c-BN), and wurtzite boron nitride. Among these, hexagonal boron nitride (h-BN) is particularly preferable. Boron nitride may be scaly primary particles or secondary particles formed by agglomeration of primary particles.
窒化ホウ素の平均粒径は、１μｍ〜４０μｍのものが好ましく、５μｍ〜２０μｍのものがより好ましく、５μｍ〜１０μｍのものがさらに好ましい。
窒化ホウ素の平均粒径は１μｍ以上であると、熱伝導率及び絶縁耐電圧が向上する傾向がある。窒化ホウ素の平均粒径が４０μｍ以下であると、粒子の形状による熱伝導率の異方性が大きくなりすぎることを抑制することができる。
The average particle size of boron nitride is preferably 1 μm to 40 μm, more preferably 5 μm to 20 μm, and even more preferably 5 μm to 10 μm.
When the average particle size of boron nitride is 1 μm or more, the thermal conductivity and the dielectric strength voltage tend to be improved. It can suppress that the anisotropy of the heat conductivity by the shape of particle | grains becomes it too large that the average particle diameter of boron nitride is 40 micrometers or less.
前記窒化ホウ素は１種類を単独で用いてもよいし、２種類以上併用してもよい。 The boron nitride may be used alone or in combination of two or more.
熱硬化性樹脂としては、例えば、ビスフェノールＡ型エポキシ樹脂、ビスフェノールＦ型エポキシ樹脂、フェノールノボラック型エポキシ樹脂、クレゾールノボラック型エポキシ樹脂のうち少なくとも１つを含むものを用いることができる。 As the thermosetting resin, for example, a resin containing at least one of bisphenol A type epoxy resin, bisphenol F type epoxy resin, phenol novolac type epoxy resin, and cresol novolac type epoxy resin can be used.
硬化促進剤としては、例えば、２−メチルイミダゾール、２−メチル−４−エチルイミダゾール等のイミダゾール触媒、トリメチルアミン等の第３級アミン化合物、三フッ化ホウ素モノエチルアミン等のルイス酸類のうち少なくとも１つを含むものを用いることができる。 Examples of the curing accelerator include at least one of imidazole catalysts such as 2-methylimidazole and 2-methyl-4-ethylimidazole, tertiary amine compounds such as trimethylamine, and Lewis acids such as boron trifluoride monoethylamine. Can be used.
無機充填材入り樹脂に用いる有機溶剤としては、例えば、メチルエチルケトン（ＭＥＫ）、メタノール、エタノール、アセトン、シクロヘキサンノン等のうち少なくとも１つを含むものを用いることができる。 As an organic solvent used for the resin with an inorganic filler, for example, a solvent containing at least one of methyl ethyl ketone (MEK), methanol, ethanol, acetone, cyclohexane, and the like can be used.
反応希釈剤としては、例えば、ビスフェノールＡ型エポキシ樹脂、ビスフェノールＦ型エポキシ樹脂、フェノールノボラック型エポキシ樹脂等のエポキシ樹脂のうち少なくとも１つを含むものを用いることができる。 As a reaction diluent, what contains at least 1 among epoxy resins, such as a bisphenol A type epoxy resin, a bisphenol F type epoxy resin, a phenol novolak type epoxy resin, can be used, for example.
＜実施例１＞
（１）無機鱗片状粒子ペーパーの作製
マイカ（粒径２．８ｍｍ以上であるマイカ片の含有率が６３質量％）を水中に分散し、抄紙機にて濾過した後、風乾させ無機鱗片状粒子ペーパーを得た。
<Example 1>
(1) Preparation of inorganic scale-like particle paper Mica (content of mica pieces having a particle size of 2.8 mm or more is 63% by mass) is dispersed in water, filtered with a paper machine, and then air-dried. I got a paper.
（２）窒化ホウ素含有樹脂の作製
熱硬化性樹脂（ダウ・ケミカル日本株式会社、商品名「Ｄ．Ｅ．Ｎ．４３８」（「Ｄ．Ｅ．Ｎ．」は、登録商標。））６５．４質量％と、硬化促進剤として三フッ化ホウ素モノエチルアミン（和光純薬工業株式会社製）２．０質量％と、有機溶剤としてメチルエチルケトン（ＭＥＫ）（和光純薬工業株式会社製）２．６質量％とを混合した。その後、窒化ホウ素３０．０質量％を加え、さらに混合し窒化ホウ素含有樹脂を得た。
なお、窒化ホウ素含有樹脂のマイカを除いた全固形分体積中の窒化ホウ素含有率は、２０体積％であった。
(2) Preparation of boron nitride-containing resin Thermosetting resin (Dow Chemical Japan Co., Ltd., trade name “D.N.438” (“D.N.” is a registered trademark)) 4 mass%, boron trifluoride monoethylamine (manufactured by Wako Pure Chemical Industries, Ltd.) 2.0 mass% as a curing accelerator, and methyl ethyl ketone (MEK) (manufactured by Wako Pure Chemical Industries, Ltd.) 2.6 as an organic solvent. The mass% was mixed. Thereafter, 30.0% by mass of boron nitride was added and further mixed to obtain a boron nitride-containing resin.
The boron nitride content in the total solid volume excluding mica of the boron nitride-containing resin was 20% by volume.
（３）プリプレグテープの作製
得られた無機充填材入り樹脂をロールコーターでガラスクロス（日東紡績株式会社製、商品名：ＷＥＡ０３Ｇ１０３）へ塗布し、前記無機鱗片状粒子ペーパーと貼り合せた。乾燥後、幅３０ｍｍに切断しプリプレグテープを得た。
(3) Preparation of prepreg tape The obtained resin with an inorganic filler was applied to a glass cloth (manufactured by Nitto Boseki Co., Ltd., trade name: WEA03G103) with a roll coater, and bonded to the inorganic scaly particle paper. After drying, it was cut into a width of 30 mm to obtain a prepreg tape.
（４）プリプレグテープの外観
上記で得たプリプレグテープは長手方向に対して樹脂が塗工されている部分と塗工されていない部分が縦筋状に現れる外観不良がなく、また、幅方向に対する塗りムラや掠れがなく外観良好であった。
(4) Appearance of the prepreg tape The prepreg tape obtained above has no appearance defect in which the part coated with the resin and the part not coated in the longitudinal direction appear in the form of vertical streaks, and the width of the prepreg tape Appearance was good with no coating unevenness or wrinkles.
（５）プリプレグテープの硬化物作製
上記で得たプリプレグテープを圧力１０ＭＰａ、１１０℃で１０分加熱成形した。その後、圧力１０ＭＰａ、１７０℃で６０分加熱成形し、プリプレグテープの硬化物を得た。
(5) Preparation of cured product of prepreg tape The prepreg tape obtained above was heat-molded at a pressure of 10 MPa and 110 ° C for 10 minutes. Then, it heat-molded for 60 minutes at the pressure of 10 MPa and 170 degreeC, and obtained the hardened | cured material of the prepreg tape.
（６）評価
上記で得たプリプレグテープ硬化物について以下の評価を行った。
(6) Evaluation The following evaluation was performed about the prepreg tape hardened | cured material obtained above.
（熱伝導率）
プリプレグテープ硬化物について、抵抗装置（ヤマヨ試験器有限会社製、商品名：ＹＳＴ−９０１Ｓ）を用いて、プリプレグテープ硬化物の熱抵抗値を測定した。得られた熱抵抗値を逆算することで熱伝導率（Ｗ／（ｍ・Ｋ））を算出した。プリプレグテープ硬化物の熱伝導率は０．５８Ｗ／（ｍ・Ｋ）であった。
(Thermal conductivity)
About the prepreg tape hardened | cured material, the thermal resistance value of the prepreg tape hardened | cured material was measured using the resistance apparatus (Yamayo Tester Co., Ltd. make, brand name: YST-901S). The thermal conductivity ( W / (m · K) ) was calculated by back-calculating the obtained thermal resistance value. The thermal conductivity of the cured prepreg tape was 0.58 W / (m · K) .
（ガラス転移温度）
プリプレグテープ硬化物について、動的粘弾性装置（Ｒｈｅｏｍｅｔｒｉｃｓ社製、商品名：Ｓｏｌｉｄ Ａｎａｌｙｚｅｒ ＲＳＡＩＩ）を用いて、プリプレグテープ硬化物のガラス転移温度（Ｔｇ値）を測定した。測定は、引っ張りモードにて、昇温速度２℃／ｍｉｎ、スパン間距離２０ｍｍで行った。
上記方法で測定したプリプレグテープ硬化物のＴｇ値は１８８℃であった。
上記評価結果を表１に示す。
(Glass-transition temperature)
About the prepreg tape hardened | cured material, the glass transition temperature (Tg value) of the prepreg tape hardened | cured material was measured using the dynamic viscoelasticity apparatus (Rheometrics company make, brand name: Solid Analyzer RSAII). The measurement was performed in a tensile mode at a temperature rising rate of 2 ° C./min and a span distance of 20 mm.
The Tg value of the cured prepreg tape measured by the above method was 188 ° C.
The evaluation results are shown in Table 1.
＜実施例２＞
（１）無機鱗片状粒子ペーパーの作製
無機鱗片状粒子ペーパーは実施例１と同様に作製した。
<Example 2>
(1) Preparation of inorganic scaly particle paper Inorganic scaly particle paper was prepared in the same manner as in Example 1.
（２）窒化ホウ素含有樹脂の作製
熱硬化性樹脂（ダウ・ケミカル日本株式会社製、商品名「Ｄ．Ｅ．Ｎ．４３８」）４２．３質量％と、硬化促進剤として三フッ化ホウ素モノエチルアミン（和光純薬工業株式会社製）１．８質量％と、有機溶剤としてメチルエチルケトン（ＭＥＫ）（和光純薬工業株式会社製）１．８質量％と、反応希釈剤としてエポキシ樹脂（ダウ・ケミカル日本株式会社製、商品名「Ｄ．Ｅ．Ｎ．４３１」）１８．１質量％を混合した。その後、窒化ホウ素３６．０質量％を加え、さらに混合し窒化ホウ素含有樹脂を得た。
なお、窒化ホウ素含有樹脂のマイカを除いた全固形分体積中の窒化ホウ素含有率は、２４体積％であった。
(2) Preparation of boron nitride-containing resin 42.3 mass% of thermosetting resin (Dow Chemical Japan, trade name “D.N.438”) and boron trifluoride mono-oxide as a curing accelerator Ethylamine (manufactured by Wako Pure Chemical Industries, Ltd.) 1.8% by mass, methyl ethyl ketone (MEK) (manufactured by Wako Pure Chemical Industries, Ltd.) 1.8% by mass as an organic solvent, and epoxy resin (Dow Chemical) as a reaction diluent 18.1% by mass (trade name “D.E.N.431”) manufactured by Nippon Co., Ltd. was mixed. Thereafter, 36.0% by mass of boron nitride was added and further mixed to obtain a boron nitride-containing resin.
The boron nitride content in the total solid volume excluding mica of the boron nitride-containing resin was 24% by volume.
（３）プリプレグテープの作製
得られた無機充填材入り樹脂をロールコーターでガラスクロス（日東紡績株式会社製、商品名：ＷＥＡ０３Ｇ１０３）へ塗布し、前記無機鱗片状粒子ペーパーと貼り合せた。乾燥後、幅３０ｍｍに切断しプリプレグテープを得た。
(3) Preparation of prepreg tape The obtained resin with an inorganic filler was applied to a glass cloth (manufactured by Nitto Boseki Co., Ltd., trade name: WEA03G103) with a roll coater, and bonded to the inorganic scaly particle paper. After drying, it was cut into a width of 30 mm to obtain a prepreg tape.
（４）プリプレグテープの外観
上記で得たプリプレグテープは長手方向に対して樹脂が塗工されている部分と塗工されていない部分が縦筋状に現れる外観不良がなく、また、幅方向に対する塗りムラや掠れがなく外観良好であった。
(4) Appearance of the prepreg tape The prepreg tape obtained above has no appearance defect in which the part coated with the resin and the part not coated in the longitudinal direction appear in the form of vertical streaks, and the width of the prepreg tape Appearance was good with no coating unevenness or wrinkles.
（５）プリプレグテープの硬化物作製
上記で得たプリプレグテープを圧力１０ＭＰａ、１１０℃で１０分加熱成形した。その後、圧力１０ＭＰａ、１７０℃で６０分加熱成形し、プリプレグテープの硬化物を得た。
(5) Preparation of cured product of prepreg tape The prepreg tape obtained above was heat-molded at a pressure of 10 MPa and 110 ° C for 10 minutes. Then, it heat-molded for 60 minutes at the pressure of 10 MPa and 170 degreeC, and obtained the hardened | cured material of the prepreg tape.
得られたプリプレグテープ硬化物について、実施例１と同様にして評価した。前記プリプレグテープ硬化物のＴｇ値は１８０℃であった。
また、前記プリプレグテープ硬化物の熱伝導率は０．６２Ｗ／（ｍ・Ｋ）であった。
上記評価結果を表１に示す。
The obtained prepreg tape cured product was evaluated in the same manner as in Example 1. The Tg value of the prepreg tape cured product was 180 ° C.
The cured prepreg tape had a thermal conductivity of 0.62 W / (m · K) .
The evaluation results are shown in Table 1.
＜比較例１＞
（１）無機鱗片状粒子ペーパーの作製
無機鱗片状粒子ペーパーは実施例１と同様に作製した。
<Comparative Example 1>
(1) Preparation of inorganic scaly particle paper Inorganic scaly particle paper was prepared in the same manner as in Example 1.
（２）無機充填材未含有樹脂の作製
熱硬化性樹脂（ダウ・ケミカル日本株式会社製、商品名「Ｄ．Ｅ．Ｎ．４３８」）９４．４質量％と、硬化促進剤として三フッ化ホウ素モノエチルアミン（和光純薬工業株式会社製）２．８質量％と、有機溶剤としてメチルエチルケトン（ＭＥＫ）（和光純薬工業株式会社製）２．８質量％とを混合し、無機充填材未含有樹脂を得た。
(2) Preparation of resin containing no inorganic filler 94.4% by mass of thermosetting resin (manufactured by Dow Chemical Japan Co., Ltd., trade name “D.N.438”) and trifluoride as a curing accelerator Boron monoethylamine (manufactured by Wako Pure Chemical Industries, Ltd.) 2.8% by mass and methyl ethyl ketone (MEK) (manufactured by Wako Pure Chemical Industries, Ltd.) 2.8% by mass as an organic solvent are mixed, and no inorganic filler is contained. A resin was obtained.
（３）プリプレグテープの作製
得られた無機充填材未含有樹脂をロールコーターでガラスクロス（日東紡績株式会社製、商品名：ＷＥＡ０３Ｇ１０３）へ塗布し、前記無機鱗片状粒子ペーパーと貼り合せた。乾燥後、幅３０ｍｍに切断しプリプレグテープを得た。
(3) Preparation of prepreg tape The obtained inorganic filler-free resin was applied to a glass cloth (manufactured by Nitto Boseki Co., Ltd., trade name: WEA03G103) with a roll coater, and bonded to the inorganic scaly particle paper. After drying, it was cut into a width of 30 mm to obtain a prepreg tape.
（４）プリプレグテープの外観
上記で得たプリプレグテープは長手方向に対して樹脂が塗工されている部分と塗工されていない部分が縦筋状に現れる外観不良がなく、また、幅方向に対する塗りムラや掠れがなく外観良好であった。
(4) Appearance of the prepreg tape The prepreg tape obtained above has no appearance defect in which the part coated with the resin and the part not coated in the longitudinal direction appear in the form of vertical streaks, and the width of the prepreg tape Appearance was good with no coating unevenness or wrinkles.
（５）プリプレグテープ硬化物の作製
上記で得たプリプレグテープを圧力１０ＭＰａ、１１０℃で１０分加熱成形した。その後、圧力１０ＭＰａ、１７０℃で６０分加熱成形し、プリプレグテープの硬化物を得た。
(5) Preparation of cured prepreg tape The prepreg tape obtained above was heat-molded at a pressure of 10 MPa and 110 ° C for 10 minutes. Then, it heat-molded for 60 minutes at the pressure of 10 MPa and 170 degreeC, and obtained the hardened | cured material of the prepreg tape.
得られたプリプレグテープ硬化物について、実施例１と同様にして評価した。前記プリプレグテープ硬化物のＴｇ値は１８８℃であった。
また、前記プリプレグテープ硬化物の熱伝導率は０．３０Ｗ／（ｍ・Ｋ）であった。
上記評価結果を表１に示す。
The obtained prepreg tape cured product was evaluated in the same manner as in Example 1. The prepreg tape cured product had a Tg value of 188 ° C.
The cured prepreg tape had a thermal conductivity of 0.30 W / (m · K) .
The evaluation results are shown in Table 1.
＜比較例２＞
（１）無機鱗片状粒子ペーパーの作製
無機鱗片状粒子ペーパーは実施例１と同様に作製した。
<Comparative Example 2>
(1) Preparation of inorganic scaly particle paper Inorganic scaly particle paper was prepared in the same manner as in Example 1.
（２）窒化ホウ素含有樹脂の作製
熱硬化性樹脂（ダウ・ケミカル日本株式会社製、商品名「Ｄ．Ｅ．Ｎ．４３８」）３３．１質量％と、硬化促進剤として三フッ化ホウ素モノエチルアミン（和光純薬工業株式会社製）１．０質量％と、有機溶剤としてメチルエチルケトン（ＭＥＫ）（和光純薬工業株式会社製）３１．９質量％とを混合した。その後、窒化ホウ素３４．０質量％を加え、さらに混合し窒化ホウ素含有樹脂を得た。
なお、窒化ホウ素含有樹脂のマイカを除いた全固形分体積中の窒化ホウ素含有率は、３５体積％であった。
(2) Preparation of boron nitride-containing resin 33.1% by mass of thermosetting resin (Dow Chemical Japan, trade name “D.E.N.438”) and boron trifluoride mono as a curing accelerator Ethylamine (manufactured by Wako Pure Chemical Industries, Ltd.) 1.0 mass% and methyl ethyl ketone (MEK) (manufactured by Wako Pure Chemical Industries, Ltd.) 31.9 mass% as an organic solvent were mixed. Thereafter, 34.0% by mass of boron nitride was added and further mixed to obtain a boron nitride-containing resin.
The boron nitride content in the total solid volume excluding mica of the boron nitride-containing resin was 35% by volume.
（３）プリプレグテープの作製
得られた窒化ホウ素含有樹脂をロールコーターでガラスクロス（日東紡績株式会社製、商品名：ＷＥＡ０３Ｇ１０３）へ塗布し、前記無機鱗片状粒子ペーパーと貼り合せた。乾燥後、幅３０ｍｍに切断しプリプレグテープを得た。
(3) Preparation of prepreg tape The obtained boron nitride-containing resin was applied to a glass cloth (manufactured by Nitto Boseki Co., Ltd., trade name: WEA03G103) with a roll coater, and bonded to the inorganic scaly particle paper. After drying, it was cut into a width of 30 mm to obtain a prepreg tape.
（４）プリプレグテープの外観
上記で得たプリプレグテープは長手方向に対して樹脂が塗工されている部分と塗工されていない部分が縦筋状に現れ外観不良であった。
(4) Appearance of prepreg tape In the prepreg tape obtained above, a portion where the resin was applied and a portion where the resin was not applied appeared in the form of vertical stripes in the longitudinal direction, and the appearance was poor.
（５）プリプレグテープ硬化物の作製
上記で得たプリプレグテープを圧力１０ＭＰａ、１１０℃で１０分加熱成形した。その後、圧力１０ＭＰａ、１７０℃で６０分加熱成形し、プリプレグテープの硬化物を得た。
(5) Preparation of cured prepreg tape The prepreg tape obtained above was heat-molded at a pressure of 10 MPa and 110 ° C for 10 minutes. Then, it heat-molded for 60 minutes at the pressure of 10 MPa and 170 degreeC, and obtained the hardened | cured material of the prepreg tape.
得られたプリプレグテープ硬化物について、実施例１と同様にして評価した。
前記プリプレグテープ硬化物のＴｇ値は１４５℃であった。
また、前記プリプレグテープ硬化物の熱伝導率は０．６４Ｗ／（ｍ・Ｋ）であった。
上記評価結果を表１に示す。
The obtained prepreg tape cured product was evaluated in the same manner as in Example 1.
The prepreg tape cured product had a Tg value of 145 ° C.
The cured prepreg tape had a thermal conductivity of 0.64 W / (m · K) .
The evaluation results are shown in Table 1.
＜比較例３＞
（１）無機鱗片状粒子ペーパーの作製
無機鱗片状粒子ペーパーは実施例１と同様に作製した。
<Comparative Example 3>
(1) Preparation of inorganic scaly particle paper Inorganic scaly particle paper was prepared in the same manner as in Example 1.
（２）窒化ホウ素含有樹脂の作製
熱硬化性樹脂（ダウ・ケミカル日本株式会社製、商品名「Ｄ．Ｅ．Ｎ．４３８」）５８．４質量％と、硬化促進剤として三フッ化ホウ素モノエチルアミン（和光純薬工業株式会社製）１．８質量％と、有機溶剤としてメチルエチルケトン（ＭＥＫ）（和光純薬工業株式会社製）５．０質量％とを混合した。その後、窒化ホウ素３４．８質量部を加え、さらに混合し窒化ホウ素含有樹脂を得た。
なお、窒化ホウ素含有樹脂のマイカを除いた全固形分体積中の窒化ホウ素含有率は、２４体積％であった。
(2) Production of boron nitride-containing resin 58.4% by mass of thermosetting resin (manufactured by Dow Chemical Japan Co., Ltd., trade name “D.E.N.438”), and boron trifluoride monohydrate as a curing accelerator 1.8% by mass of ethylamine (manufactured by Wako Pure Chemical Industries, Ltd.) and 5.0% by mass of methyl ethyl ketone (MEK) (manufactured by Wako Pure Chemical Industries, Ltd.) as an organic solvent were mixed. Thereafter, 34.8 parts by mass of boron nitride was added and further mixed to obtain a boron nitride-containing resin.
The boron nitride content in the total solid volume excluding mica of the boron nitride-containing resin was 24% by volume.
（３）プリプレグテープの作製
得られた窒化ホウ素含有樹脂をロールコーターでガラスクロス（日東紡績株式会社製、商品名：ＷＥＡ０３Ｇ１０３）へ塗布し、前記無機鱗片状粒子ペーパーと貼り合せた。乾燥後、幅３０ｍｍに切断しプリプレグテープを得た。
(3) Preparation of prepreg tape The obtained boron nitride-containing resin was applied to a glass cloth (manufactured by Nitto Boseki Co., Ltd., trade name: WEA03G103) with a roll coater, and bonded to the inorganic scaly particle paper. After drying, it was cut into a width of 30 mm to obtain a prepreg tape.
（４）プリプレグテープの外観
上記で得たプリプレグテープは長手方向に対して樹脂が塗工されている部分と塗工されていない部分が縦筋状に現れる外観不良はなく、また、幅方向に対する塗りムラや掠れがなく外観良好であった。
(4) Appearance of prepreg tape In the prepreg tape obtained above, there is no appearance defect in which a portion coated with resin and a portion not coated with respect to the longitudinal direction appear in the form of vertical streaks, and the width in the width direction Appearance was good with no coating unevenness or wrinkles.
（５）プリプレグテープ硬化物の作製
上記で得たプリプレグテープを圧力１０ＭＰａ、１１０℃で１０分加熱成形した。その後、圧力１０ＭＰａ、１７０℃で６０分加熱成形し、プリプレグテープの硬化物を得た。
(5) Preparation of cured prepreg tape The prepreg tape obtained above was heat-molded at a pressure of 10 MPa and 110 ° C for 10 minutes. Then, it heat-molded for 60 minutes at the pressure of 10 MPa and 170 degreeC, and obtained the hardened | cured material of the prepreg tape.
得られたプリプレグテープ硬化物について、実施例１と同様にして評価した。
前記プリプレグテープ硬化物のＴｇ値は１５５℃であった。
また、前記プリプレグテープ硬化物の熱伝導率は０．６１Ｗ／（ｍ・Ｋ）であった。
上記評価結果を表１に示す。
The obtained prepreg tape cured product was evaluated in the same manner as in Example 1.
The prepreg tape cured product had a Tg value of 155 ° C.
The cured prepreg tape had a thermal conductivity of 0.61 W / (m · K) .
The evaluation results are shown in Table 1.
図１に実施例１、２及び比較例２、３のプリプレグテープを表す断面の概略図を示す。図２に比較例１のプリプレグテープを表す断面の概略図を示す。図３に実施例のプリプレグテープの製造方法についてのフローチャートを示す。
図１、２において、符号１は窒化ホウ素粒子、符号２は裏打ち材を、符号３は熱硬化性樹脂を、符号４はマイカを、各々表す。
The schematic of the cross section showing the prepreg tapes of Examples 1 and 2 and Comparative Examples 2 and 3 is shown in FIG. The schematic of the cross section showing the prepreg tape of the comparative example 1 is shown in FIG. The flowchart about the manufacturing method of the prepreg tape of an Example is shown in FIG.
1 and 2,
表１より、本発明によれば、有機溶剤量を減らしたプリプレグテープは高い熱伝導率を有しつつ、１８０℃以上の高い耐熱性を有する外観良好なプリプレグテープを得ることができることが明らかである。
また、有機溶剤量を減らし、反応希釈剤を加えることで窒化ホウ素の充填量を増やすことが可能で、０．６Ｗ／（ｍ・Ｋ）以上の熱伝導率を有しつつ、１８０℃以上の高い耐熱性を有する外観良好なプリプレグテープを得ることができることが明らかである。
From Table 1, it is clear that according to the present invention, a prepreg tape with a reduced amount of organic solvent can obtain a prepreg tape with high heat conductivity of 180 ° C. or higher and good appearance while having high thermal conductivity. is there.
Moreover, it is possible to increase the filling amount of boron nitride by reducing the amount of organic solvent and adding a reaction diluent, and having a thermal conductivity of 0.6 W / (m · K) or more, 180 ° C. or more It is apparent that a prepreg tape having high heat resistance and good appearance can be obtained.
１ 無機充填材（窒化ホウ素粒子）
２ 裏打ち材
３ 熱硬化性樹脂
４ 無機鱗片状粒子（マイカ）
1 Inorganic filler (boron nitride particles)
2
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| JPS5435399A (en) * | 1977-08-24 | 1979-03-15 | Hitachi Ltd | Preparing mica sheet |
| JPS6016691B2 (en) * | 1977-11-02 | 1985-04-26 | 株式会社日立製作所 | Manufacturing method of prepreg insulation tape |
| JPS58207604A (en) * | 1982-05-28 | 1983-12-03 | Toshiba Corp | Electrically-insulated coil and manufacture thereof |
| SE455246B (en) * | 1986-10-22 | 1988-06-27 | Asea Ab | MANUFACTURER FOR SAVING IN A STATOR OR ROTOR IN AN ELECTRIC MACHINE AND MANUFACTURING A MANUFACTURING |
| US5633042A (en) * | 1996-05-28 | 1997-05-27 | Matsushita Electric Works, Ltd. | Process for manufacturing prepregs for use as electric insulating material |
| JP2000173818A (en) * | 1998-12-02 | 2000-06-23 | Hitachi Ltd | Coil and manufacture of coil |
| JP2000210962A (en) * | 1999-01-26 | 2000-08-02 | Matsushita Electric Works Ltd | Manufacture of laminate |
| JP5598190B2 (en) * | 2010-09-09 | 2014-10-01 | 住友ベークライト株式会社 | Thermosetting resin composition for circuit board |
| JP2012244861A (en) * | 2011-05-24 | 2012-12-10 | Mitsubishi Electric Corp | Insulation coil |
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