JP2679449B2 - Semiconductor porcelain having positive temperature coefficient of resistance and manufacturing method thereof - Google Patents
Semiconductor porcelain having positive temperature coefficient of resistance and manufacturing method thereofInfo
- Publication number
- JP2679449B2 JP2679449B2 JP3141083A JP14108391A JP2679449B2 JP 2679449 B2 JP2679449 B2 JP 2679449B2 JP 3141083 A JP3141083 A JP 3141083A JP 14108391 A JP14108391 A JP 14108391A JP 2679449 B2 JP2679449 B2 JP 2679449B2
- Authority
- JP
- Japan
- Prior art keywords
- resistance
- tisi
- temperature coefficient
- positive temperature
- semiconductor
- 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.)
- Expired - Lifetime
Links
- 239000004065 semiconductor Substances 0.000 title claims description 42
- 229910052573 porcelain Inorganic materials 0.000 title claims description 22
- 238000004519 manufacturing process Methods 0.000 title claims description 7
- 229910008484 TiSi Inorganic materials 0.000 claims description 22
- 239000000463 material Substances 0.000 claims description 20
- 239000000919 ceramic Substances 0.000 claims description 15
- 238000002441 X-ray diffraction Methods 0.000 claims description 13
- 229910002113 barium titanate Inorganic materials 0.000 claims description 12
- JRPBQTZRNDNNOP-UHFFFAOYSA-N barium titanate Chemical compound [Ba+2].[Ba+2].[O-][Ti]([O-])([O-])[O-] JRPBQTZRNDNNOP-UHFFFAOYSA-N 0.000 claims description 12
- 239000002245 particle Substances 0.000 claims description 12
- 238000010304 firing Methods 0.000 claims description 2
- 238000001354 calcination Methods 0.000 claims 1
- 230000003068 static effect Effects 0.000 description 13
- 230000015556 catabolic process Effects 0.000 description 9
- 238000000034 method Methods 0.000 description 8
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 4
- 239000000203 mixture Substances 0.000 description 4
- 239000004698 Polyethylene Substances 0.000 description 2
- 239000003795 chemical substances by application Substances 0.000 description 2
- -1 polyethylene Polymers 0.000 description 2
- 229920000573 polyethylene Polymers 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 229910010413 TiO 2 Inorganic materials 0.000 description 1
- 229910052788 barium Inorganic materials 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 229910010293 ceramic material Inorganic materials 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 238000000465 moulding Methods 0.000 description 1
- 238000010298 pulverizing process Methods 0.000 description 1
- 229910052761 rare earth metal Inorganic materials 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
Landscapes
- Compositions Of Oxide Ceramics (AREA)
- Silicon Compounds (AREA)
- Apparatuses And Processes For Manufacturing Resistors (AREA)
- Thermistors And Varistors (AREA)
Description
【発明の詳細な説明】DETAILED DESCRIPTION OF THE INVENTION
【０００１】[0001]
【産業上の利用分野】本願発明は、正の抵抗温度係数を
有するチタン酸バリウム（ＢａＴｉＯ3）系半導体磁器
に関し、詳しくは、高い静耐圧を有する半導体磁器及び
その製造方法に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a barium titanate (BaTiO 3 ) based semiconductor ceramic having a positive temperature coefficient of resistance, and more particularly to a semiconductor ceramic having a high static breakdown voltage and a method for manufacturing the same.
【０００２】[0002]
【従来の技術】近年、大きな正の抵抗温度係数を有する
チタン酸バリウム（ＢａＴｉＯ3）系半導体磁器が開発
されており、この半導体磁器は、キュリー温度を越える
と抵抗値が急激に増大して、通過する電流量を減少させ
ることから、回路の過電流保護用や、テレビ受像機のブ
ラウン管枠の消磁用など種々の用途に広く用いられてい
る。一方、このチタン酸バリウム系半導体磁器を用いた
素子の信頼性を向上させるために、より静耐圧の高い正
の抵抗温度係数を有する半導体磁器に対する要求が高ま
っている。2. Description of the Related Art In recent years, barium titanate (BaTiO 3 ) based semiconductor porcelain having a large positive temperature coefficient of resistance has been developed, and the resistance of this semiconductor porcelain rapidly increases when the Curie temperature is exceeded. Since it reduces the amount of current passing through, it is widely used for various purposes such as circuit overcurrent protection and degaussing of the cathode ray tube frame of a television receiver. On the other hand, in order to improve the reliability of an element using this barium titanate-based semiconductor ceramic, there is an increasing demand for a semiconductor ceramic having a positive resistance temperature coefficient with a higher static breakdown voltage.
【０００３】従来、チタン酸バリウム系半導体磁器の静
耐圧を向上させる方法として、半導体化剤を含んだＢａ
ＴｉＯ3系材料に、平均組成Ｂａ2ＴｉＳｉ2Ｏ8で表され
る成分材料を添加して焼成する方法が提案されている
（特開昭６２−２９６４０１号公報）。Conventionally, as a method for improving the static breakdown voltage of barium titanate-based semiconductor ceramics, Ba containing a semiconducting agent has been used.
A method has been proposed in which a component material represented by the average composition Ba 2 TiSi 2 O 8 is added to a TiO 3 -based material and fired (JP-A-62-296401).
【０００４】[0004]
【発明が解決しようとする課題】しかし、上記従来の方
法では、半導体磁器の静耐圧をある程度向上させること
はできるが、その効果は必ずしも十分ではないという問
題点があり、さらに静耐圧の高い半導体磁器及びその製
造方法が求められている。However, although the conventional method described above can improve the static breakdown voltage of the semiconductor porcelain to some extent, there is a problem that the effect is not always sufficient. There is a need for porcelain and methods of making the same.
【０００５】本願発明は、上記問題点を解決するもので
あり、従来の半導体磁器よりも静耐圧に優れた正の抵抗
温度係数を有する半導体磁器及びその製造方法を提供す
ることを目的とする。The present invention solves the above problems, and an object of the present invention is to provide a semiconductor porcelain having a positive temperature coefficient of resistance which is more excellent in static breakdown voltage than the conventional semiconductor porcelain, and a method for manufacturing the same.
【０００６】[0006]
【課題を解決するための手段】上記目的を達成するため
に、本願発明の正の抵抗温度係数を有する半導体磁器
は、チタン酸バリウム系半導体材料にＢａ2ＴｉＳｉ2Ｏ
8を添加し焼成した正の抵抗温度係数を有するチタン酸
バリウム系半導体磁器であって、該半導体磁器焼成体の
中心部のＢａ2ＴｉＳｉ2Ｏ8（１，１，１）面のＸ線回
折強度Ｉｎと、該半導体磁器焼成体の表面部のＢａ2Ｔ
ｉＳｉ2Ｏ8（１，１，１）面のＸ線回折強度Ｉｓとの比
Ｉｎ／Ｉｓが７以上であることを特徴とする。In order to achieve the above object, a semiconductor ceramic having a positive temperature coefficient of resistance of the present invention is a barium titanate-based semiconductor material containing Ba 2 TiSi 2 O.
A barium titanate-based semiconductor porcelain having a positive temperature coefficient of resistance obtained by adding 8 to the sintered body, and the Ba 2 TiSi 2 O 8 (1,1,1) plane at the center of the sintered body of the semiconductor porcelain is subjected to X-ray diffraction. Strength In and Ba 2 T of the surface portion of the semiconductor ceramic fired body
The ratio In / Is of the iSi 2 O 8 (1,1,1) plane to the X-ray diffraction intensity Is is 7 or more.
【０００７】また、本願発明の正の抵抗温度係数を有す
る半導体磁器の製造方法は、チタン酸バリウム系半導体
材料にＢａ2ＴｉＳｉ2Ｏ8を添加した混合材料を平均粒
径が３μm以下になるまで粉砕し、これを焼成すること
を特徴とする。Further, the method for manufacturing a semiconductor ceramic having a positive temperature coefficient of resistance according to the present invention is a method for preparing a mixed material obtained by adding Ba 2 TiSi 2 O 8 to a barium titanate-based semiconductor material until the average particle diameter becomes 3 μm or less. It is characterized in that it is crushed and fired.
【０００８】発明者らは、正の抵抗温度係数を有する半
導体磁器の静耐圧をさらに向上させるべく鋭意検討を行
い、ＢａＴｉＯ3系半導体磁器材料にフレスナイト（Ｂ
ａ2ＴｉＳｉ2Ｏ8）を添加して焼成した半導体磁器焼成
体中のＢａ2ＴｉＳｉ2Ｏ8の分布状態が静耐圧に重要な
関係を有することを知り、本願発明を完成させるに至っ
た。すなわち、本願発明半導体磁器においては、ＢａＴ
ｉＯ3系半導体磁器材料の仮焼粉にＢａ2ＴｉＳｉ2Ｏ8を
添加し、これを平均粒径が３μm以下になるまで粉砕し
た後、焼成することにより、焼成体（半導体磁器）の中
心部のＢａ2ＴｉＳｉ2Ｏ8の分布密度が表面部よりも高
くなり、静耐圧が向上する。そして、上記のようにして
得られる半導体磁器焼成体の、中心部のＢａ2ＴｉＳｉ2
Ｏ8（１，１，１）面のＸ線回折強度Ｉｎと、該半導体
磁器焼成体の表面部のＢａ2ＴｉＳｉ2Ｏ8（１，１，
１）面のＸ線回折強度Ｉｓとの比Ｉｎ／Ｉｓは７以上に
なる。The inventors of the present invention have made earnest studies to further improve the static withstand voltage of a semiconductor ceramic having a positive temperature coefficient of resistance, and have used Fresnite (B) as a BaTiO 3 -based semiconductor ceramic material.
It was found that the distribution state of Ba 2 TiSi 2 O 8 in the sintered body of the semiconductor porcelain fired by adding a 2 TiSi 2 O 8 ) has an important relationship with the static breakdown voltage, and the present invention has been completed. That is, in the semiconductor ceramic of the present invention, BaT
Ba 2 TiSi 2 O 8 was added to the calcined powder of the iO 3 -based semiconductor porcelain material, and this was crushed until the average particle size became 3 μm or less, and then calcined to obtain the center part of the calcined body (semiconductor porcelain). Distribution density of Ba 2 TiSi 2 O 8 is higher than that of the surface portion, and the static breakdown voltage is improved. Then, the Ba 2 TiSi 2 in the central portion of the semiconductor ceramic fired body obtained as described above is used.
O 8 (1, 1, 1) and X-ray diffraction intensity In the surface, the semiconductor ceramic fired body of the surface portion of the Ba 2 TiSi 2 O 8 (1,1 ,
The ratio In / Is of the 1) plane to the X-ray diffraction intensity Is is 7 or more.
【０００９】[0009]
【実施例】以下に、実施例を示して本願発明の特徴をさ
らに詳細に説明する。EXAMPLES The features of the present invention will be described in more detail below with reference to examples.
【００１０】ＢａＣＯ3，ＴｉＯ2，Ｙ2Ｏ3，ＣａＣ
Ｏ3、Ｍｎ2Ｏ3を下記の式(1)で表される組成になるよう
に調合する。 （Ｂａ0.896Ｃａ0.10Ｙ0.004）ＴｉＯ3＋0.0005Ｍｎ ……(1) そして、これを純水及びジルコニアボールとともにポリ
エチレン製ポットに入れて５時間粉砕混合した後、乾燥
し、１１５０℃で２時間仮焼する。この仮焼粉に１モル
％のＢａ2ＴｉＳｉ2Ｏ8を添加して下記の式(2)の組成の
混合材料を調合する。 ［(Ｂａ0.896Ｃａ0.10Ｙ0.004)ＴｉＯ3＋0.0005Ｍｎ]＋0.01Ｂａ2ＴｉＳｉ2Ｏ8 ……(2)BaCO 3 , TiO 2 , Y 2 O 3 , CaC
O 3 and Mn 2 O 3 are prepared so as to have a composition represented by the following formula (1). (Ba 0.896 Ca 0.10 Y 0.004 ) TiO 3 +0.0005 Mn (1) Then, put this together with pure water and zirconia balls in a polyethylene pot, pulverize and mix for 5 hours, dry, and temporarily store at 1150 ° C. for 2 hours. Bake. 1 mol% of Ba 2 TiSi 2 O 8 is added to the calcined powder to prepare a mixed material having the composition of the following formula (2). [(Ba 0.896 Ca 0.10 Y 0.004 ) TiO 3 +0.0005 Mn] +0.01 Ba 2 TiSi 2 O 8 (2)
【００１１】これをポリエチレン製ポットに入れ、バイ
ンダを添加するとともに、ジルコニアボール及び純水を
入れて粉砕混合を行う。これにより、混合材料の平均粒
径を０．５〜５μmの範囲で変化させ、Ｂａ2ＴｉＳｉ2
Ｏ8の分布制御を行う。それから、このスラリーを乾
燥、造粒し、プレス成形機により直径１７mm、厚さ１mm
の円板状の成形体を作成する。そして、この成形体を、
８℃／minの割合で１３５０℃にまで昇温し、その温度
で３０分間焼成し、さらに８℃／minの割合で室温にま
で冷却して焼成体（半導体磁器）を作成した。それか
ら、この半導体磁器の両主面に、電極材料を塗布して電
極を形成し、特性測定のための試料とした。This is placed in a polyethylene pot, a binder is added, and zirconia balls and pure water are placed and pulverized and mixed. As a result, the average particle size of the mixed material is changed within the range of 0.5 to 5 μm, and Ba 2 TiSi 2
The distribution control of O 8 is performed. Then, this slurry is dried, granulated, and pressed by a press molding machine to have a diameter of 17 mm and a thickness of 1 mm.
A disk-shaped molded body of is prepared. And this molded body,
The temperature was raised to 1350 ° C. at a rate of 8 ° C./min, firing was performed at that temperature for 30 minutes, and further cooled to room temperature at a rate of 8 ° C./min to produce a fired body (semiconductor porcelain). Then, electrode materials were applied to both main surfaces of this semiconductor porcelain to form electrodes, which were used as samples for characteristic measurement.
【００１２】表１に、上記実施例の試料についての、Ｂ
ａ2ＴｉＳｉ2Ｏ8を混合粉砕した後の混合材料の平均粒
径、半導体磁器の中心部のＢａ2ＴｉＳｉ2Ｏ8（１，
１，１）面のＸ線回折強度Ｉｎと表面部のＢａ2ＴｉＳ
ｉ2Ｏ8（１，１，１）面のＸ線回折強度Ｉｓの比Ｉｎ／
Ｉｓ、常温（２５℃）における抵抗、及び静耐圧（素子
に印加される電圧を上昇させた場合に電流が最小値にな
る電圧値）の各値を示す。Table 1 shows the B of the samples of the above examples.
The average particle size of the mixed material after mixing and crushing a 2 TiSi 2 O 8 and Ba 2 TiSi 2 O 8 (1,
X-ray diffraction intensity In of the 1,1) plane and Ba 2 TiS of the surface portion
The ratio In / of the X-ray diffraction intensity Is of the i 2 O 8 (1,1,1) plane
Each value of Is, resistance at room temperature (25 ° C.), and static withstand voltage (voltage value at which current becomes minimum value when voltage applied to element is increased) is shown.
【００１３】[0013]
【表１】 [Table 1]
【００１４】なお、表１において、＊印を付した試料は
本願発明の範囲外のものである。表１より、混合材料の
平均粒径を３μm以下にすることにより、中心部と表面
部のＸ線回折強度比Ｉｎ／Ｉｓの値が７以上になり、平
均粒径が０．５μmになるとＩｎ／Ｉｓの値は３６とな
っている。また、Ｘ線回折強度比Ｉｎ／Ｉｓの値が７以
上（すなわち、混合材料の平均粒径が３μm以下）にな
ると半導体磁器の静耐圧は７０Ｖを越えており、著しく
向上していることがわかる。また、Ｉｎ／Ｉｓがそれ以
上大きくなっても静耐圧はそれほど急激には向上せず、
Ｉｎ／Ｉｓが３６（平均粒径０．５μm）のときに８１
Ｖとなっている。したがって、Ｘ線回折強度比Ｉｎ／Ｉ
ｓは７以上にすることが好ましい。In Table 1, the samples marked with * are outside the scope of the present invention. From Table 1, by setting the average particle diameter of the mixed material to 3 μm or less, the value of the X-ray diffraction intensity ratio In / Is of the central portion and the surface portion becomes 7 or more, and when the average particle diameter becomes 0.5 μm, In The value of / Is is 36. Further, when the value of the X-ray diffraction intensity ratio In / Is is 7 or more (that is, the average particle diameter of the mixed material is 3 μm or less), the static withstand voltage of the semiconductor porcelain exceeds 70 V, which is remarkably improved. . Further, even if In / Is becomes larger than that, the static breakdown voltage does not sharply improve,
81 when In / Is is 36 (average particle size 0.5 μm)
V. Therefore, the X-ray diffraction intensity ratio In / I
It is preferable that s is 7 or more.
【００１５】一方、比抵抗は、混合材料の平均粒径のい
かんにかかわらず、ほぼ一定（０．８３〜０．８７Ω）
であり、混合材料の平均粒径（すなわち、Ｉｎ／Ｉｓの
値）の影響を受けないことがわかる。On the other hand, the specific resistance is almost constant (0.83 to 0.87Ω) regardless of the average particle size of the mixed material.
Therefore, it is understood that the average particle size of the mixed material (that is, the value of In / Is) is not affected.
【００１６】なお、本願発明の製造方法にかかる正の抵
抗温度係数を有する半導体磁器の主成分であるチタン酸
バリウム系半導体材料としては、Ｂａの一部をＣａなど
で置換したり、さらに、半導体化剤として、Ｙなどの希
土類元素やＮｂ，Ｓｂなどの元素を含有させたりした種
々のチタン酸バリウム系材料を用いることが可能であ
る。As the barium titanate-based semiconductor material which is the main component of the semiconductor porcelain having a positive temperature coefficient of resistance according to the manufacturing method of the present invention, a part of Ba may be replaced with Ca or the like, and As the agent, various barium titanate-based materials containing a rare earth element such as Y or an element such as Nb or Sb can be used.
【００１７】[0017]
【発明の効果】上述のように、本願発明の正の抵抗温度
係数を有する半導体磁器は、その中心部と表面部のＢａ
2ＴｉＳｉ2Ｏ8のＸ線回折強度の比Ｉｎ／Ｉｓが７以上
になるようにしているので、磁器の低抵抗を保持しつ
つ、静耐圧を向上させることができる。As described above, the semiconductor porcelain having a positive temperature coefficient of resistance according to the present invention has Ba at the center and the surface thereof.
Since the ratio In / Is of the X-ray diffraction intensity of 2 TiSi 2 O 8 is set to 7 or more, the static resistance can be improved while maintaining the low resistance of the porcelain.
【００１８】また、本願発明の正の抵抗温度係数を有す
る半導体磁器の製造方法は、ＢａＴｉＯ3系半導体材料
にＢａ2ＴｉＳｉ2Ｏ8を混合して粉砕した混合材料の平
均粒径が３μm以下になるように粒度調整し、これを焼
成するようにしているので、Ｂａ2ＴｉＳｉ2Ｏ8の分布
を、上記Ｘ線回折強度比Ｉｎ／Ｉｓの値が７以上になる
ように制御することが可能になり、静耐圧に優れた正の
抵抗温度係数を有する半導体磁器を得ることができる。Further, in the method for manufacturing a semiconductor ceramic having a positive temperature coefficient of resistance according to the present invention, the average particle diameter of the mixed material obtained by mixing Ba 2 TiSi 2 O 8 with BaTiO 3 type semiconductor material and pulverizing it is 3 μm or less. Since the grain size is adjusted so that it is baked, it is possible to control the distribution of Ba 2 TiSi 2 O 8 so that the value of the above X-ray diffraction intensity ratio In / Is is 7 or more. As a result, it is possible to obtain a semiconductor ceramic having a positive temperature coefficient of resistance which is excellent in static breakdown voltage.
───────────────────────────────────────────────────── フロントページの続き (56)参考文献 特開 昭62−296401（ＪＰ，Ａ) 特開 昭64−22001（ＪＰ，Ａ) 特開 昭58−24842（ＪＰ，Ａ) ─────────────────────────────────────────────────── ─── Continuation of the front page (56) References JP 62-296401 (JP, A) JP 64-22001 (JP, A) JP 58-24842 (JP, A)
Claims (2)
ＴｉＳｉ2Ｏ8を添加し焼成した正の抵抗温度係数を有す
るチタン酸バリウム系半導体磁器であって、該半導体磁
器焼成体の中心部のＢａ2ＴｉＳｉ2Ｏ8（１，１，１）
面のＸ線回折強度Ｉｎと、該半導体磁器焼成体の表面部
のＢａ2ＴｉＳｉ2Ｏ8（１，１，１）面のＸ線回折強度
Ｉｓとの比Ｉｎ／Ｉｓが７以上であることを特徴とする
正の抵抗温度係数を有する半導体磁器。1. A barium titanate-based semiconductor material containing Ba 2
A barium titanate-based semiconductor porcelain having a positive temperature coefficient of resistance obtained by adding TiSi 2 O 8 and firing, wherein Ba 2 TiSi 2 O 8 (1,1,1) is present at the center of the fired body of the semiconductor porcelain.
The ratio In / Is of the X-ray diffraction intensity In of the surface and the X-ray diffraction intensity Is of the Ba 2 TiSi 2 O 8 (1,1,1) surface of the surface portion of the semiconductor porcelain calcination body is 7 or more. A semiconductor porcelain having a positive temperature coefficient of resistance.
ＴｉＳｉ2Ｏ8を添加した混合材料を平均粒径が３μm以
下になるまで粉砕し、これを焼成することを特徴とする
請求項１記載の正の抵抗温度係数を有する半導体磁器の
製造方法。2. A barium titanate-based semiconductor material containing Ba 2
The method for producing a semiconductor ceramic having a positive temperature coefficient of resistance according to claim 1, characterized in that the mixed material to which TiSi 2 O 8 is added is crushed until the average particle diameter becomes 3 μm or less and then fired.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP3141083A JP2679449B2 (en) | 1991-05-15 | 1991-05-15 | Semiconductor porcelain having positive temperature coefficient of resistance and manufacturing method thereof |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP3141083A JP2679449B2 (en) | 1991-05-15 | 1991-05-15 | Semiconductor porcelain having positive temperature coefficient of resistance and manufacturing method thereof |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH04338601A JPH04338601A (en) | 1992-11-25 |
| JP2679449B2 true JP2679449B2 (en) | 1997-11-19 |
Family
ID=15283816
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP3141083A Expired - Lifetime JP2679449B2 (en) | 1991-05-15 | 1991-05-15 | Semiconductor porcelain having positive temperature coefficient of resistance and manufacturing method thereof |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2679449B2 (en) |
Families Citing this family (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6071842A (en) * | 1997-09-05 | 2000-06-06 | Tdk Corporation | Barium titanate-based semiconductor ceramic |
| JP4080576B2 (en) * | 1997-09-05 | 2008-04-23 | Ｔｄｋ株式会社 | Method for manufacturing positive characteristic semiconductor porcelain |
| JP4058140B2 (en) * | 1997-09-05 | 2008-03-05 | Ｔｄｋ株式会社 | Barium titanate semiconductor porcelain |
-
1991
- 1991-05-15 JP JP3141083A patent/JP2679449B2/en not_active Expired - Lifetime
Also Published As
| Publication number | Publication date |
|---|---|
| JPH04338601A (en) | 1992-11-25 |
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