JPH04288337A - Composite high-molecular dielectric material - Google Patents
Composite high-molecular dielectric materialInfo
- Publication number
- JPH04288337A JPH04288337A JP257191A JP257191A JPH04288337A JP H04288337 A JPH04288337 A JP H04288337A JP 257191 A JP257191 A JP 257191A JP 257191 A JP257191 A JP 257191A JP H04288337 A JPH04288337 A JP H04288337A
- Authority
- JP
- Japan
- Prior art keywords
- filler
- dielectric constant
- titanate
- fibers
- perovskite
- Prior art date
- 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.)
- Granted
Links
- 239000002131 composite material Substances 0.000 title claims description 21
- 239000003989 dielectric material Substances 0.000 title claims description 7
- 239000000835 fiber Substances 0.000 claims abstract description 33
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims abstract description 24
- 239000000945 filler Substances 0.000 claims abstract description 19
- 229910052751 metal Inorganic materials 0.000 claims abstract description 15
- 239000002184 metal Substances 0.000 claims abstract description 15
- 239000011159 matrix material Substances 0.000 claims abstract description 8
- 229910052788 barium Inorganic materials 0.000 claims abstract description 7
- 229910052791 calcium Inorganic materials 0.000 claims abstract description 6
- 229910052749 magnesium Inorganic materials 0.000 claims abstract description 6
- 229910052712 strontium Inorganic materials 0.000 claims abstract description 6
- 229910052745 lead Inorganic materials 0.000 claims abstract description 5
- 229920000642 polymer Polymers 0.000 claims description 10
- 239000003513 alkali Substances 0.000 claims description 9
- 239000002952 polymeric resin Substances 0.000 claims description 5
- 229920003002 synthetic resin Polymers 0.000 claims description 5
- -1 titanate compound Chemical class 0.000 claims description 4
- 229910010252 TiO3 Inorganic materials 0.000 claims 1
- 229910052698 phosphorus Inorganic materials 0.000 claims 1
- 229920005989 resin Polymers 0.000 abstract description 5
- 239000011347 resin Substances 0.000 abstract description 5
- 239000000463 material Substances 0.000 abstract description 4
- 238000000034 method Methods 0.000 description 7
- 239000007864 aqueous solution Substances 0.000 description 4
- 238000001027 hydrothermal synthesis Methods 0.000 description 4
- JRPBQTZRNDNNOP-UHFFFAOYSA-N barium titanate Chemical compound [Ba+2].[Ba+2].[O-][Ti]([O-])([O-])[O-] JRPBQTZRNDNNOP-UHFFFAOYSA-N 0.000 description 3
- 229910002113 barium titanate Inorganic materials 0.000 description 3
- 239000003990 capacitor Substances 0.000 description 3
- 239000000919 ceramic Substances 0.000 description 3
- 229920001707 polybutylene terephthalate Polymers 0.000 description 3
- 239000002861 polymer material Substances 0.000 description 3
- 150000001875 compounds Chemical class 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 239000010410 layer Substances 0.000 description 2
- 238000000465 moulding Methods 0.000 description 2
- 239000008188 pellet Substances 0.000 description 2
- 239000002344 surface layer Substances 0.000 description 2
- 239000010936 titanium Substances 0.000 description 2
- VXUYXOFXAQZZMF-UHFFFAOYSA-N titanium(IV) isopropoxide Chemical compound CC(C)O[Ti](OC(C)C)(OC(C)C)OC(C)C VXUYXOFXAQZZMF-UHFFFAOYSA-N 0.000 description 2
- 150000004703 alkoxides Chemical class 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- RQPZNWPYLFFXCP-UHFFFAOYSA-L barium dihydroxide Chemical compound [OH-].[OH-].[Ba+2] RQPZNWPYLFFXCP-UHFFFAOYSA-L 0.000 description 1
- 229910001863 barium hydroxide Inorganic materials 0.000 description 1
- CPUJSIVIXCTVEI-UHFFFAOYSA-N barium(2+);propan-2-olate Chemical compound [Ba+2].CC(C)[O-].CC(C)[O-] CPUJSIVIXCTVEI-UHFFFAOYSA-N 0.000 description 1
- 229910010293 ceramic material Inorganic materials 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 239000000805 composite resin Substances 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- NJLLQSBAHIKGKF-UHFFFAOYSA-N dipotassium dioxido(oxo)titanium Chemical compound [K+].[K+].[O-][Ti]([O-])=O NJLLQSBAHIKGKF-UHFFFAOYSA-N 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000010304 firing Methods 0.000 description 1
- 230000005484 gravity Effects 0.000 description 1
- 238000007731 hot pressing Methods 0.000 description 1
- 230000001771 impaired effect Effects 0.000 description 1
- 238000001746 injection moulding Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 239000004033 plastic Substances 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 238000003980 solgel method Methods 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 238000004544 sputter deposition Methods 0.000 description 1
- 229920005992 thermoplastic resin Polymers 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 238000001771 vacuum deposition Methods 0.000 description 1
Landscapes
- Processes Of Treating Macromolecular Substances (AREA)
- Manufacture Of Macromolecular Shaped Articles (AREA)
- Reinforced Plastic Materials (AREA)
- Injection Moulding Of Plastics Or The Like (AREA)
Abstract
Description
【０００１】0001
【産業上の利用分野】 本発明は、コンデンサ等に利
用される高分子複合誘電体に関する。TECHNICAL FIELD The present invention relates to a polymer composite dielectric material used in capacitors and the like.
【０００２】0002
【従来の技術】 高分子材料の誘電率はほぼ５以下で
あり、コンデンサの小型化や大容量化に対応できなかっ
た。コンデンサあるいは高誘電率を必要とする用途に対
応するために、樹脂自体の高誘電率化を行う方法、ある
いは誘電率の大きいセラミックスの粉体や繊維をフィラ
ーとしてプラスチック等からなるマトリックスに分散し
複合化を行う方法の、大別して２つの試みがなされてい
る。後者の方法では、樹脂とセラミックスを複合化した
際の体積率Ｎ１ ，Ｎ２，およびそれぞれの誘電率ε１
，ε２ により、複合材の誘電率εは、
ｌｏｇε＝Ｎ１ ｌｏｇε１ ＋Ｎ２ ｌｏｇε２ ・
・・・（１）により与えられる。（１）式より明らかな
ように、誘電率の大きい一方の物質の体積率を高くする
ことにより、誘電率を向上させることができ、そのよう
な試みがなされてきた。[Prior Art] The dielectric constant of polymeric materials is approximately 5 or less, and it has not been possible to respond to miniaturization and increase in capacitance of capacitors. In order to respond to capacitors and other applications that require a high dielectric constant, there are methods to increase the dielectric constant of the resin itself, or composites in which ceramic powder or fiber with a high dielectric constant is dispersed as a filler in a matrix made of plastic, etc. Broadly speaking, two approaches have been made to achieve this. In the latter method, the volume fractions N1 and N2 and the dielectric constants ε1 of the composite resin and ceramics are
, ε2, the dielectric constant ε of the composite material is: logε=N1 logε1 +N2 logε2 ・
...Given by (1). As is clear from Equation (1), the dielectric constant can be improved by increasing the volume fraction of one of the materials having a large dielectric constant, and such attempts have been made.
【０００３】0003
【発明が解決しようとする課題】 ところが、上述し
たように従来技術では高誘電率を得るために、セラミッ
クスフィラーを高い体積率で充填することにより、複合
材の誘電率を向上することができるものの、体積率を高
くすると樹脂本来の性質が損なわれる熱可塑性樹脂など
では、成型方法が限定されるという問題がある。したが
って、この両者を満足した実用的な複合量では、高分子
材料の誘電率がセラミックス材料に比べ小さいため、比
誘電率が２０程度の複合材料しか得られていなかった。[Problem to be Solved by the Invention] However, as described above, in the conventional technology, in order to obtain a high dielectric constant, the dielectric constant of the composite material can be improved by filling the ceramic filler at a high volume ratio. For thermoplastic resins, etc., in which the inherent properties of the resin are impaired when the volume fraction is increased, there is a problem in that molding methods are limited. Therefore, in a practical composite amount that satisfies both of these requirements, only a composite material with a dielectric constant of about 20 has been obtained because the dielectric constant of the polymer material is smaller than that of the ceramic material.
【０００４】本発明は、従来のチタン酸バリウム繊維を
フィラーとする複合材料に比べ少ないフィラーの体積率
で高誘電率特性が得られる高分子複合材料を提供するこ
とを目的とする。[0004] An object of the present invention is to provide a polymer composite material that can obtain high dielectric constant properties with a smaller filler volume fraction than conventional composite materials containing barium titanate fibers as fillers.
【０００５】[0005]
【課題を解決するための手段】 本発明の目的を達成
するために、本発明の高分子複合誘電体は、Ｃａ、Ｓｒ
、Ｂａ、ＭｇおよびＰｂのうち少なくとも一種以上のＡ
群元素からなるＡＴｉＯ３−Ｘ （０＜ｘ＜３）で表さ
れるペロブスカイト型のチタン酸金属塩繊維を、高分子
樹脂からなるマトリックス中に分散されてなることによ
って特徴づけられる。[Means for Solving the Problems] In order to achieve the objects of the present invention, the polymer composite dielectric of the present invention has Ca, Sr,
, Ba, Mg, and Pb.
It is characterized in that perovskite-type metal titanate fibers represented by ATiO3-X (0<x<3) consisting of group elements are dispersed in a matrix made of a polymer resin.
【０００６】また、導電性または半導電性のチタン酸ア
ルカリ繊維、またはそのチタン酸アルカリ繊維から誘導
されたチタン酸繊維に、Ｃａ、Ｓｒ、Ｂａ、Ｍｇおよび
Ｐｂのうち、少なくとも一種以上のＡ群元素からなる、
ＡＴｉＯ３ で表されるペロブスカイト型チタン酸金属
塩化合物の皮膜が形成されたフィラーが、高分子樹脂か
らなるマトリックス中に分散されてなることによって特
徴づけられる。[0006] In addition, conductive or semiconductive alkali titanate fibers or titanate fibers derived from the alkali titanate fibers may contain at least one member of Group A selected from Ca, Sr, Ba, Mg, and Pb. consisting of elements,
It is characterized in that a filler on which a film of a perovskite metal titanate compound represented by ATiO3 is formed is dispersed in a matrix made of a polymer resin.
【０００７】[0007]
【作用】 中心部が導電性または半導電性のチタン酸
アルカリ繊維またはチタン酸アルカリ繊維からの誘導さ
れたチタン酸繊維からなり、表面層が主にＣａ、Ｓｒ、
Ｂａ、ＭｇおよびＰｂのうち、少なくとも一種以上のＡ
群元素からなるＡＴｉＯ３ で表されるペロブスカイト
型チタン酸金属塩化合物からなる二層構造を有している
。繊維を高分子材料に複合した高分子複合誘電体は、図
３に示す等価回路で表される複合材料となり、見かけの
誘電率を大きくすることができる。[Function] The center part consists of conductive or semiconductive alkali titanate fibers or titanate fibers derived from alkali titanate fibers, and the surface layer mainly consists of Ca, Sr,
At least one type of A among Ba, Mg and Pb
It has a two-layer structure consisting of a perovskite-type titanate metal salt compound represented by ATiO3 consisting of group elements. A polymer composite dielectric material made by combining fibers with a polymer material becomes a composite material represented by the equivalent circuit shown in FIG. 3, and can have a large apparent dielectric constant.
【０００８】またＡＴｉＯ３−Ｘ （０＜ｘ＜３）繊維
を高分子材料に複合化した場合も、従来の酸素欠陥のな
いＡＴｉＯ３ 繊維を複合化した場合より大きな誘電率
の複合材料が得られる。Also, when ATiO3-X (0<x<3) fibers are composited with a polymer material, a composite material with a higher dielectric constant can be obtained than when conventional ATiO3 fibers without oxygen vacancies are composited.
【０００９】[0009]
【実施例】 図１は本発明実施例の斜視図である。本
発明実施例の高分子複合誘電体３は、高分子樹脂からな
るマトリックス２にＡＴｉＯ３−Ｘ （０＜ｘ＜３）で
表されるフィラー１が複合されている。フィラー１であ
るＡＴｉＯ３−Ｘ （０＜ｘ＜３）なるペロブスカイト
型チタン酸金属塩繊維は、還元して得られる導電性また
は半導電性のチタン酸アルカリ繊維やチタン酸繊維を、
その繊維に含まれるチタンと等量以上のＡなる金属元素
であるＢａ等の二価金属を含む水溶液中で常圧または水
熱反応することによりえられる。Embodiment FIG. 1 is a perspective view of an embodiment of the present invention. In the polymer composite dielectric material 3 of the embodiment of the present invention, a filler 1 represented by ATiO3-X (0<x<3) is composited into a matrix 2 made of a polymer resin. The filler 1, ATiO3-X (0<x<3), is a perovskite metal titanate fiber, which is obtained by reducing conductive or semiconductive alkali titanate fiber or titanate fiber.
It can be obtained by a normal pressure or hydrothermal reaction in an aqueous solution containing a divalent metal such as Ba, which is a metal element A, in an amount equal to or more than titanium contained in the fiber.
【００１０】図２は本発明実施例の二層構造を有するフ
ィラーの斜視図である。このフィラーは、中心部は導電
性チタン酸アルカリ繊維１ａからなり、表面層にはＡＴ
ｉＯ３−Ｘ （０＜ｘ＜３）で表されるチタン酸金属塩
１ｂが形成されている。また、皮膜の形成は、■ 導
電性または半導電性のチタン酸アルカリ繊維やチタン酸
繊維を水酸化バリウム等の二価の金属を含む水溶液中で
常圧または水熱反応させる。■ バリウムイソプロポ
キシドや二価金属のアルコキシドとチタンイソプロポキ
シドの溶液に繊維を浸漬する等の、いわゆるゾルーゲル
法。■ スパッタ等の真空蒸着法。等の方法で実現で
きる。FIG. 2 is a perspective view of a filler having a two-layer structure according to an embodiment of the present invention. The center of this filler is made of conductive alkali titanate fiber 1a, and the surface layer is made of AT.
A metal titanate salt 1b represented by iO3-X (0<x<3) is formed. The film is formed by (1) subjecting conductive or semiconductive titanate alkali fibers or titanate fibers to a normal pressure or hydrothermal reaction in an aqueous solution containing a divalent metal such as barium hydroxide. ■ So-called sol-gel methods, such as immersing fibers in solutions of barium isopropoxide, divalent metal alkoxides, and titanium isopropoxide. ■ Vacuum deposition methods such as sputtering. This can be achieved using the following methods.
【００１１】本発明実施例では、上述のうち■による方
法でフィラーを形成した。すなわち、還元焼成によって
造られた比抵抗１０４ 程度程度のチタン酸カリウム繊
維を、繊維に含まれるＴｉに対して１．２のＢａを含む
水溶液中で水熱反応させることによりＢａＴｉＯ３−Ｘ
繊維を、同じく０．７５のＢａを含む水溶液中で水熱
反応させることによりＢａＴｉＯ３−Ｘ 皮膜を形成し
た。これらの繊維をフィラーとしてＰＢＴ（ポリブチレ
ンテレフタレート）樹脂に対して２０〜４０％の体積率
で、押し出し機を用い溶融および混合することにより、
コンパウンドペレットを作製した。なお、比重はＰＢＴ
が１．３１、フィラー繊維は４．７である。このコンパ
ウンドペレットを用いて、ホットプレスにより所定寸法
の成型板を作製して、誘電率、誘電損失、体積抵抗率を
測定した結果を表１に示す。In the examples of the present invention, fillers were formed by the method (2) above. That is, by subjecting potassium titanate fibers produced by reduction firing and having a specific resistance of about 104 to a hydrothermal reaction in an aqueous solution containing 1.2% Ba to Ti contained in the fibers, BaTiO3-X
A BaTiO3-X film was formed by subjecting the fiber to a hydrothermal reaction in an aqueous solution containing 0.75 Ba. By using an extruder to melt and mix these fibers as fillers at a volume ratio of 20 to 40% with respect to PBT (polybutylene terephthalate) resin,
Compound pellets were produced. In addition, the specific gravity is PBT
is 1.31, and the filler fiber is 4.7. Using this compound pellet, a molded plate of predetermined dimensions was produced by hot pressing, and the dielectric constant, dielectric loss, and volume resistivity were measured. Table 1 shows the results.
【００１２】0012
【表１】[Table 1]
【００１３】なお、比較例は本発明者らが先に出願して
いる特願平２−１１３４４４（未公開）により作製した
チタン酸バリウム繊維を本発明実施例と同条件で混合し
た複合材料を用いた測定結果である。なお、測定にあた
っては、誘電率およびｔａｎδは１ＭＨｚでの測定値、
また体積抵抗率は５００Ｖでの測定値である。 表１
から明らかなように、本発明実施例では、その誘電損失
は従来例と同等であり、また、誘電率は従来例のほぼ１
．５〜２倍となった。とくに、その誘電率は３０以上と
いう、これまで得ることができなかった値を有する高分
子複合誘電体が得られた効果は大きい。[0013] The comparative example is a composite material obtained by mixing barium titanate fibers produced in accordance with Japanese Patent Application No. 2-113444 (unpublished) previously filed by the present inventors under the same conditions as the examples of the present invention. These are the measurement results used. In addition, when measuring, the dielectric constant and tan δ are measured values at 1 MHz,
Moreover, the volume resistivity is a value measured at 500V. Table 1
As is clear from the above, in the embodiment of the present invention, the dielectric loss is the same as that of the conventional example, and the dielectric constant is approximately 1 of that of the conventional example.
．． It became 5 to 2 times. In particular, the effect of obtaining a polymer composite dielectric material having a dielectric constant of 30 or more, a value that could not be obtained until now, is significant.
【００１４】[0014]
【発明の効果】 以上説明したように、本発明によれ
ば、従来のチタン酸バリウム繊維の複合材料に比べ少な
いフィラーの添加量で高誘電率特性が得られる高分子複
合材料を提供することができる。また、フィラーの充填
率の低い高分子複合材料であるから、従来のように樹脂
本来の性質が損なわれることにより成型方法が限定され
るということもなく、たとえば射出成形が可能なことか
ら、複雑な形状のものでも簡単な製造工程で作製できる
効果もある。[Effects of the Invention] As explained above, according to the present invention, it is possible to provide a polymer composite material that can obtain high dielectric constant characteristics with a smaller amount of filler added than conventional barium titanate fiber composite materials. can. In addition, since it is a polymer composite material with a low filler filling rate, there are no limitations on molding methods due to loss of the original properties of the resin, as is the case with conventional methods, and injection molding is possible, making it less complex. It also has the advantage that it can be manufactured with a simple manufacturing process even if it has a small shape.
【図１】 本発明実施例の斜視図[Fig. 1] Perspective view of an embodiment of the present invention
【図２】 本発明実施例のフィラーの斜視図[Figure 2] Perspective view of the filler according to the embodiment of the present invention
【図３】
本発明実施例の等価回路[Figure 3]
Equivalent circuit of the embodiment of the present invention
１・・・・フィラー １ａ・・・・チタン酸アルカリ繊維 １ｂ・・・・チタン酸金属塩 ２・・・・マトリックス ３・・・・高分子複合誘電体 1... Filler 1a... Alkaline titanate fiber 1b...Metal titanate salt 2...Matrix 3...Polymer composite dielectric material
Claims (2)
うち少なくとも一種以上のＡ群元素からなるＡＴｉＯ３
−Ｘ （０＜ｘ＜３）で表されるペロブスカイト型のチ
タン酸金属塩繊維を、高分子樹脂からなるマトリックス
中に分散されてなる高分子複合誘電体。[Claim 1] ATiO3 consisting of at least one group A element among Ca, Sr, Ba, Mg and Pb.
-X (0<x<3) perovskite-type metal titanate fibers are dispersed in a matrix made of a polymer resin.
カリ繊維、またはそのチタン酸アルカリ繊維から誘導さ
れたチタン酸繊維に、Ｃａ、Ｓｒ、Ｂａ、ＭｇおよびＰ
ｂのうち、少なくとも一種以上のＡ群元素からなる、Ａ
ＴｉＯ３ で表されるペロブスカイト型チタン酸金属塩
化合物の皮膜が形成されたフィラーが、高分子樹脂から
なるマトリックス中に分散されてなる高分子複合誘電体
。2. Conductive or semiconductive alkali titanate fibers, or titanate fibers derived from the alkali titanate fibers, containing Ca, Sr, Ba, Mg and P.
A consisting of at least one group A element among b
A polymer composite dielectric material in which a filler on which a film of a perovskite metal titanate compound represented by TiO3 is formed is dispersed in a matrix made of a polymer resin.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP3002571A JP2530943B2 (en) | 1991-01-14 | 1991-01-14 | Polymer composite dielectric |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP3002571A JP2530943B2 (en) | 1991-01-14 | 1991-01-14 | Polymer composite dielectric |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH04288337A true JPH04288337A (en) | 1992-10-13 |
| JP2530943B2 JP2530943B2 (en) | 1996-09-04 |
Family
ID=11533058
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP3002571A Expired - Lifetime JP2530943B2 (en) | 1991-01-14 | 1991-01-14 | Polymer composite dielectric |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2530943B2 (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2017511426A (en) * | 2014-03-28 | 2017-04-20 | サン−ゴバン サントル ドゥ ルシェルシェ エ デトゥードゥ ユーロペン | Polymer-ceramic composite material |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH03281574A (en) * | 1990-03-29 | 1991-12-12 | Otsuka Chem Co Ltd | Highly dielectric resin composition |
-
1991
- 1991-01-14 JP JP3002571A patent/JP2530943B2/en not_active Expired - Lifetime
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH03281574A (en) * | 1990-03-29 | 1991-12-12 | Otsuka Chem Co Ltd | Highly dielectric resin composition |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2017511426A (en) * | 2014-03-28 | 2017-04-20 | サン−ゴバン サントル ドゥ ルシェルシェ エ デトゥードゥ ユーロペン | Polymer-ceramic composite material |
Also Published As
| Publication number | Publication date |
|---|---|
| JP2530943B2 (en) | 1996-09-04 |
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