JPS6147914B2 - - Google Patents
Info
- Publication number
- JPS6147914B2 JPS6147914B2 JP59168881A JP16888184A JPS6147914B2 JP S6147914 B2 JPS6147914 B2 JP S6147914B2 JP 59168881 A JP59168881 A JP 59168881A JP 16888184 A JP16888184 A JP 16888184A JP S6147914 B2 JPS6147914 B2 JP S6147914B2
- Authority
- JP
- Japan
- Prior art keywords
- hydrochloric acid
- salt water
- pipe
- dispersion
- dispersion tube
- 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
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- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 110
- 150000003839 salts Chemical class 0.000 claims description 56
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 54
- 239000006185 dispersion Substances 0.000 claims description 44
- 238000000034 method Methods 0.000 claims description 17
- 238000005868 electrolysis reaction Methods 0.000 claims description 16
- 239000011148 porous material Substances 0.000 claims description 7
- 235000002639 sodium chloride Nutrition 0.000 description 51
- 239000012267 brine Substances 0.000 description 7
- HPALAKNZSZLMCH-UHFFFAOYSA-M sodium;chloride;hydrate Chemical compound O.[Na+].[Cl-] HPALAKNZSZLMCH-UHFFFAOYSA-M 0.000 description 7
- 238000005260 corrosion Methods 0.000 description 5
- 230000007797 corrosion Effects 0.000 description 5
- 238000010586 diagram Methods 0.000 description 5
- 239000004810 polytetrafluoroethylene Substances 0.000 description 5
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 5
- 239000000463 material Substances 0.000 description 4
- 239000002253 acid Substances 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 239000003014 ion exchange membrane Substances 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- 229920006395 saturated elastomer Polymers 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 238000005341 cation exchange Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- -1 hydroxyl ions Chemical class 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 239000011780 sodium chloride Substances 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
Landscapes
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Description
【発明の詳細な説明】
〔産業上の利用分野〕
本発明は電解槽への塩酸添加方法に関するもの
であつて、具体的には食塩等の塩化アルカリ水溶
液の電解に際して、陽極液PHを下げるために行わ
れる塩酸添加の方法に関するものである。[Detailed Description of the Invention] [Industrial Application Field] The present invention relates to a method for adding hydrochloric acid to an electrolytic cell, and specifically, for lowering the pH of an anolyte during electrolysis of an aqueous alkali chloride solution such as common salt. This relates to a method of adding hydrochloric acid to
食塩等のアルカリ電解の技術分野において、
種々の利点から、隔膜に陽イオン交換膜を用いる
いわゆるイオン交換膜法アルカリ電解が主流にな
りつつあるが、電解中、陰極室からイオン交換膜
を通つて陽極室に拡散してくる水酸イオン
（OH-）を速やかに中和することが必要であり、
そのために酸添加して陽極液のPHを下げることが
よく行なわれている。酸として一般的に用いられ
るのは塩酸であるが、この塩酸を具体的に陽極液
に添加する手段としてはいろいろな方法が考えら
れている。その主なものとして、電解槽から排水
される陽極液の気液分離器に塩酸を供給する方法
や、陽極室に塩水を供給する配管中に、細いパイ
プから直接に塩酸を投入する方法等がある。
In the technical field of alkaline electrolysis for salt etc.
Due to various advantages, the so-called ion exchange membrane alkaline electrolysis using a cation exchange membrane as a diaphragm is becoming mainstream, but during electrolysis, hydroxyl ions diffuse from the cathode chamber through the ion exchange membrane to the anode chamber. It is necessary to quickly neutralize (OH - ),
For this reason, it is common practice to lower the pH of the anolyte by adding acid. Although hydrochloric acid is generally used as an acid, various methods have been considered for specifically adding this hydrochloric acid to the anolyte. The main methods include a method of supplying hydrochloric acid to a gas-liquid separator for the anolyte drained from the electrolytic cell, and a method of directly injecting hydrochloric acid from a thin pipe into the piping that supplies salt water to the anode chamber. be.
ここに用いられる塩酸は、通常濃塩酸であつ
て、上記いずれの場合も気液分離器や配管を腐食
させやすいという欠点がある。 The hydrochloric acid used here is usually concentrated hydrochloric acid, and in any of the above cases, it has the disadvantage that it tends to corrode the gas-liquid separator and piping.
本発明は、電解槽に塩酸を添加する際に従来問
題となつていた塩酸による装置材料の腐食を防止
しうる方法を提供するものである。
The present invention provides a method that can prevent corrosion of equipment materials due to hydrochloric acid, which has conventionally been a problem when adding hydrochloric acid to an electrolytic cell.
本発明者等は、塩水供給配管中に塩酸を供給す
る場合に、上述の如き塩酸による腐食の問題が生
じないような具体的方法について種々検討した結
果本発明を見出したもので、本発明は、塩水配管
中の電解用塩水に塩酸を供給して電解槽に塩酸を
添加する方法において、塩酸の細流を流出しうる
細孔を有する分散管を塩水配管のほぼ中心線に沿
つて配置し、該分散管に塩酸を供給することを特
徴とする電解槽への塩酸添加法を要旨とするもの
である。
The present inventors have discovered the present invention as a result of various studies on specific methods that do not cause the above-mentioned corrosion problem due to hydrochloric acid when supplying hydrochloric acid into salt water supply piping. In a method of adding hydrochloric acid to an electrolytic salt water in a salt water pipe and adding it to an electrolytic cell, a dispersion pipe having a pore through which a trickle of hydrochloric acid can flow is arranged approximately along the center line of the salt water pipe, The gist of this invention is a method of adding hydrochloric acid to an electrolytic cell, which is characterized by supplying hydrochloric acid to the dispersion tube.
以下、図面をもとに本発明を説明する。第１図
は、本発明に好適に用いられうる分散管の１例を
示す見取図である。第２図は、第１図の分散管を
塩水配管に配置した時の塩酸の流水の状態を示す
断面図である。 The present invention will be explained below based on the drawings. FIG. 1 is a sketch showing one example of a dispersion tube that can be suitably used in the present invention. FIG. 2 is a cross-sectional view showing the state of hydrochloric acid flowing when the dispersion pipe shown in FIG. 1 is placed in a salt water pipe.
第１図に示される分散管は、先端が円錐状に閉
じられた管の側壁の多数の細孔が設けられたもの
である。分散管の上方から供給される塩酸は細孔
を通じて四囲に流出する。その流出の状態を示す
ものが第２図である。塩水配管のほぼ中心線に沿
つて配置された分散管には上方より塩酸が、一
方、塩水配管と分散管の間には塩水が供給され
る。分散管に供給される塩酸は、その側壁に設け
られた細孔を通つて塩水配管を流れている塩水中
に流出する。塩水中に流出した塩酸は、分散管の
外側面に沿いつつ、分散管の下方へ行くにつれて
ややふくらみを増しながらも、塩水配管の内壁と
は接触しないように、ほぼ塩水配管の中心線上を
流下していく。 The dispersion tube shown in FIG. 1 is a tube with a closed conical tip and a large number of pores in the side wall. Hydrochloric acid supplied from above the dispersion tube flows out to the surrounding area through the pores. FIG. 2 shows the state of the outflow. Hydrochloric acid is supplied from above to the dispersion pipe arranged approximately along the center line of the salt water pipe, while salt water is supplied between the salt water pipe and the dispersion pipe. Hydrochloric acid supplied to the dispersion tube flows out through pores provided in its side wall into the salt water flowing through the salt water piping. The hydrochloric acid that has flowed into the salt water flows along the outer surface of the dispersion pipe, bulging slightly as it goes downwards, but flows down almost on the center line of the salt water pipe so as not to come into contact with the inner wall of the salt water pipe. I will do it.
かくして、本発明方法によれば、材料的には少
量の分散管にのみ耐塩酸性の材料を用いれば、大
量の材料を要する塩水配管には、耐塩酸性を要求
されない安価な材質ものが使用可能となる。本発
明において、分散管の開孔は、そこから流出する
塩酸の流速が電解用塩水の流速と同じか、それ以
下となるような断面積を有するものであることが
好ましい。ここで、分散管から流出する塩酸の流
速とは、分散管に供給される塩酸の体積速度を開
孔の総面積で除したものを意味する。 Thus, according to the method of the present invention, by using a hydrochloric acid resistant material only for a small amount of the dispersion tube, inexpensive materials that are not required to be hydrochloric acid resistant can be used for salt water piping that requires a large amount of material. Become. In the present invention, the openings of the dispersion tube preferably have a cross-sectional area such that the flow rate of hydrochloric acid flowing out from the openings is the same as or lower than the flow rate of the electrolytic brine. Here, the flow rate of hydrochloric acid flowing out from the dispersion tube means the volumetric velocity of hydrochloric acid supplied to the dispersion tube divided by the total area of the openings.
また。電解用塩水の流速とは、塩水配管を流れ
る塩水の体積速度を、塩水配管の断面積と分散管
の断面積の差で除したものを意味する。 Also. The flow rate of salt water for electrolysis means the volumetric velocity of salt water flowing through the salt water pipe divided by the difference between the cross-sectional area of the salt water pipe and the cross-sectional area of the dispersion pipe.
分散管に設けられる開孔の断面積が上記限定を
満足する場合には、流出塩酸が配管と接触する可
能性が少ないため、より好ましいものである。 It is more preferable if the cross-sectional area of the opening provided in the dispersion tube satisfies the above limitations, since there is less possibility that the effluent hydrochloric acid will come into contact with the piping.
さらに、本発明においては、分散管から流出し
た塩酸は、前述の如く、塩水配管のほぼ中心線に
沿つて流動していき、徐々に四囲の塩水中に拡散
していくものであるため、中心線付近の塩酸濃度
がまだ高い状態での流路変更、即ち、塩水配管に
ベント、、ブランチ等があることは好ましくな
く、分散管の先端からある距離は塩水配管は真直
ぐであることが好ましい。 Furthermore, in the present invention, as mentioned above, the hydrochloric acid flowing out from the dispersion tube flows approximately along the center line of the salt water pipe and gradually diffuses into the surrounding salt water. It is not preferable to change the flow path while the hydrochloric acid concentration near the line is still high, that is, to have a vent, branch, etc. in the salt water pipe, and it is preferable that the salt water pipe be straight for a certain distance from the tip of the dispersion pipe.
この範囲は、前述の分散管に設けられる開孔の
断面積及び塩水の体積速度と塩酸の体積速度の比
にもよるが、最低0.2ｍあることが好ましい。 This range is preferably at least 0.2 m, although it depends on the cross-sectional area of the openings provided in the above-mentioned dispersion tube and the ratio of the volume velocity of salt water to the volume velocity of hydrochloric acid.
また、分散管先端から電解槽までの塩水配管の
長さがさして長くないような場合には、塩水配管
の電解槽直前の部分にデイストリビユーター用の
混合羽根を設けるのが安全である。 Furthermore, if the length of the salt water piping from the tip of the dispersion tube to the electrolytic cell is not very long, it is safe to provide a mixing blade for the distributor in the portion of the salt water piping immediately in front of the electrolytic cell.
また、本発明では、塩酸は分散管に供給され、
そこから塩酸配管に供給されるものであるが、分
散管には塩酸と共に一部の塩水も同時に供給する
のが、分散管中で塩酸のプレミツクスが行われる
ことから好ましい方法である。 Further, in the present invention, hydrochloric acid is supplied to the dispersion tube,
From there, the hydrochloric acid is supplied to the piping, and it is a preferable method to simultaneously supply hydrochloric acid and some brine to the dispersion tube, since premixing of hydrochloric acid is carried out in the dispersion tube.
かくして、本発明を採用する場合には、塩酸に
よる配管の腐食問題は生じなく、充分に目的を達
成できるものである。
Thus, when the present invention is employed, the problem of corrosion of piping due to hydrochloric acid does not occur, and the objective can be fully achieved.
以下、実施例により、本発明を更に詳しく説明
する。 Hereinafter, the present invention will be explained in more detail with reference to Examples.
実施例 １
第３図は、本実施例に使用した電解プラントの
塩水供給部分の拡大断面図である。精製された飽
和塩水溶液は、ブラインボツクスに４m3/hで供
給される。一方、塩酸（濃度10N）はブラインボ
ツクスの上部から、分散管に接続する内径15mmの
PTFE製パイプに25/hで供給される、塩水供給
配管（Ti製、内径125mm）は図示の如くブライン
ボツクスの底部に取りつけられ、その対端は電解
槽下部にその側方から接続されている。Example 1 FIG. 3 is an enlarged sectional view of the salt water supply part of the electrolysis plant used in this example. The purified saturated salt aqueous solution is fed to the brine box at 4 m 3 /h. On the other hand, hydrochloric acid (concentration 10N) was introduced from the top of the brine box into a 15mm inner diameter tube connected to the dispersion tube.
The salt water supply pipe (made of Ti, inner diameter 125 mm), which is supplied to the PTFE pipe at a rate of 25/h, is attached to the bottom of the brine box as shown in the diagram, and its opposite end is connected to the bottom of the electrolytic cell from the side. .
一方、分散管は外径60mm、内径50mmのPTFE製
パイプの先端が閉じられたもので、その側面に均
一に直径10mm及び直径20mmの開孔各々16個及び４
個が分散管の長手方向150mmにわたつて設けられ
ている。また、分散管下端から塩水配管のベント
部までの距離は600mmである。 On the other hand, the dispersion tube is a PTFE pipe with an outer diameter of 60 mm and an inner diameter of 50 mm, with the tip closed, and there are 16 holes each with a diameter of 10 mm and 4 holes with a diameter of 20 mm uniformly on the side of the pipe.
150 mm in the longitudinal direction of the dispersion tube. Furthermore, the distance from the lower end of the dispersion tube to the vent part of the salt water piping was 600 mm.
また、電解槽から排出される淡塩水がブライン
ボツクスに15m3/h及び塩水配管の、電解槽に供
給される直前の水平部分に、循環塩水として15
m3/hで供給される。従つて、分散管のある塩水
配管部分を流れる塩水速度は19m3/hであるが、
塩水の１部は分散管にも流出するため分散管に外
側を流れる塩水の流速は約0.55m/secである。ま
た、分散管の上記開孔から流出する希釈された塩
酸の流速は約0.55m/secである。 In addition, the fresh salt water discharged from the electrolyzer is placed in the brine box at a rate of 15 m 3 /h, and the salt water piping is placed in the horizontal section just before being supplied to the electrolyzer as circulating brine.
Supplied at m 3 /h. Therefore, the velocity of salt water flowing through the part of the salt water piping where the dispersion pipe is located is 19 m 3 /h.
A portion of the salt water also flows into the dispersion pipe, so the flow velocity of the salt water flowing outside the dispersion pipe is approximately 0.55 m/sec. Further, the flow rate of diluted hydrochloric acid flowing out from the above-mentioned opening of the dispersion tube is about 0.55 m/sec.
以上の装置、条件で電解を実施した所、電解槽
にはPH1.7の電解用塩水が供給され、図示された
塩水配管は塩酸による腐食は全く生じず、安全に
長期間電解が実施できた。 When electrolysis was carried out using the above equipment and conditions, salt water for electrolysis with a pH of 1.7 was supplied to the electrolytic cell, and the salt water piping shown in the diagram was not corroded by hydrochloric acid at all, and electrolysis could be carried out safely for a long period of time. .
実施例 ２
第３図の電解プラントにおいて、実施例１と同
様にブラインボツクス底部の塩水供給配管（Ti
製、内径125mm）に外径25mm、内径15mmのPTFE
製パイプを入れ分散管の上部に挿入する。分散管
は外径80mm、内径70mmのPTFE製パイプで先端部
が円錐状に閉じられたもので、その側面に直径10
mmの開孔24個が分散管の長手方向200mmに千鳥配
列に設けられている。また、分散管下端から塩水
配管のベント部までの距離は550mmである。飽和
塩水及び淡塩水の供給の仕方及び量は実施例１と
同じである。塩水の流速は約0.7m/secである。
一方塩酸は濃度10Nで30/hで内径15mmのPTFE
製パイプから分散管を経由して供給される。ま
た、希釈された塩酸の流速は約0.16m/secであ
る。Example 2 In the electrolysis plant shown in Figure 3, the salt water supply pipe (Ti
Made of PTFE (inner diameter 125mm), outer diameter 25mm, inner diameter 15mm
Insert the manufactured pipe into the top of the dispersion pipe. The dispersion tube is a PTFE pipe with an outer diameter of 80 mm and an inner diameter of 70 mm, the tip of which is closed in a conical shape.
24 mm-sized openings were provided in a staggered arrangement in a 200 mm longitudinal direction of the dispersion tube. Furthermore, the distance from the lower end of the dispersion pipe to the vent part of the salt water piping was 550 mm. The method and amount of supply of saturated salt water and fresh salt water are the same as in Example 1. The flow velocity of salt water is approximately 0.7 m/sec.
On the other hand, hydrochloric acid has a concentration of 10N and a PTFE with an inner diameter of 15mm at 30/h.
It is supplied from a manufactured pipe via a dispersion pipe. Furthermore, the flow velocity of diluted hydrochloric acid is approximately 0.16 m/sec.
以上の装置、条件で電解を実施したところ、電
解槽にはPH1.6の電解用塩水が供給され、図示さ
れた塩水配管は塩酸による腐食は全く見られず、
安定的に長期間電解が実施できた。 When electrolysis was carried out using the above equipment and conditions, salt water for electrolysis with a pH of 1.6 was supplied to the electrolytic cell, and the salt water piping shown in the diagram showed no corrosion due to hydrochloric acid.
Electrolysis could be carried out stably for a long period of time.
比較例 １
実施例１において、分散管を用いず内径15mmの
パイプから直接塩酸を塩水配管に供給すること以
外は、実施例１と同様にして電解実験を行なつ
た。Comparative Example 1 An electrolysis experiment was carried out in the same manner as in Example 1, except that hydrochloric acid was directly supplied to the salt water piping from a pipe with an inner diameter of 15 mm without using a dispersion tube.
結果は、塩酸供給端から、らせん状に塩水配管
の内面に腐食跡がみられた。 The results showed that corrosion marks were observed on the inner surface of the salt water pipe in a spiral pattern starting from the hydrochloric acid supply end.
これは、塩酸の流れが第４図に示すような状態
になつていることに起因するものと思われる。 This is thought to be due to the flow of hydrochloric acid being in the state shown in Figure 4.
第１図は本発明に用いられうる分散管の１例を
示す見取図である。第２図は第１図の分散管を塩
水配管に配管した時の塩酸の流れの状態を示す断
面説明図である。第３図は実施例１で使用した電
解プラントの塩水供給部分の拡大断面図である。
第４図は比較例１における塩酸の流れの状態を示
す断面説明図である。
FIG. 1 is a sketch showing one example of a dispersion tube that can be used in the present invention. FIG. 2 is a cross-sectional explanatory diagram showing the state of flow of hydrochloric acid when the dispersion pipe shown in FIG. 1 is connected to a salt water pipe. FIG. 3 is an enlarged sectional view of the salt water supply portion of the electrolysis plant used in Example 1.
FIG. 4 is an explanatory cross-sectional diagram showing the state of flow of hydrochloric acid in Comparative Example 1.
Claims (1)
解槽に塩酸を添加する方法において、塩酸の細流
を流出しうる細孔を有する分散管を塩水配管のほ
ぼ中心線に沿つて配置し、該分散管に塩酸を供給
することを特徴とする電解槽への塩酸添加法。 ２ 塩水配管は、その中心線が、分散管の先端よ
り少なくとも0.2ｍ真直ぐである特許請求の範囲
第１項記載の電解槽への塩酸添加法。 ３ 分散管の細孔は、そこから流出する塩酸の流
速が電解用塩水の流速と同じかそれ以下となる断
面積を有するものである特許請求の範囲第１項記
載の電解槽への塩酸添加法。 ４ 分散管には、塩酸とともに、一部の塩水をも
供給するものである特許請求の範囲第１項記載の
電解槽への塩酸添加法。[Claims] 1. In a method of supplying hydrochloric acid to salt water for electrolysis in a salt water pipe and adding the hydrochloric acid to an electrolytic cell, a dispersion pipe having pores through which a trickle of hydrochloric acid can flow is placed approximately at the center line of the salt water pipe. A method for adding hydrochloric acid to an electrolytic cell, characterized by supplying hydrochloric acid to the dispersion tube. 2. The method for adding hydrochloric acid to an electrolytic cell according to claim 1, wherein the center line of the salt water piping is at least 0.2 m straight from the tip of the dispersion tube. 3. Addition of hydrochloric acid to the electrolytic cell according to claim 1, wherein the pores of the dispersion tube have a cross-sectional area such that the flow rate of hydrochloric acid flowing out from the pores is the same as or lower than the flow rate of the electrolytic salt water. Law. 4. The method for adding hydrochloric acid to an electrolytic cell according to claim 1, wherein a part of salt water is also supplied to the dispersion tube along with hydrochloric acid.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59168881A JPS6148587A (en) | 1984-08-14 | 1984-08-14 | Method for adding hydrochloric acid to electrolytic cell |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59168881A JPS6148587A (en) | 1984-08-14 | 1984-08-14 | Method for adding hydrochloric acid to electrolytic cell |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS6148587A JPS6148587A (en) | 1986-03-10 |
| JPS6147914B2 true JPS6147914B2 (en) | 1986-10-21 |
Family
ID=15876289
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP59168881A Granted JPS6148587A (en) | 1984-08-14 | 1984-08-14 | Method for adding hydrochloric acid to electrolytic cell |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS6148587A (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH0540818Y2 (en) * | 1987-03-13 | 1993-10-15 |
Families Citing this family (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2627101B2 (en) * | 1990-09-19 | 1997-07-02 | 株式会社オムコ | Additive chemicals for the production of electrolytic hypochlorous acid sterilized water |
| US7727374B2 (en) * | 2004-09-23 | 2010-06-01 | Skyonic Corporation | Removing carbon dioxide from waste streams through co-generation of carbonate and/or bicarbonate minerals |
| EP3094401A4 (en) | 2014-01-17 | 2017-08-09 | Skyonic Corporation | Acid gas removal from a gaseous stream |
| EP3261991B9 (en) | 2015-02-23 | 2023-11-15 | Carbonfree Chemicals Holdings, LLC | Carbon dioxide sequestration with magnesium hydroxide and regeneration of magnesium hydroxide |
-
1984
- 1984-08-14 JP JP59168881A patent/JPS6148587A/en active Granted
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH0540818Y2 (en) * | 1987-03-13 | 1993-10-15 |
Also Published As
| Publication number | Publication date |
|---|---|
| JPS6148587A (en) | 1986-03-10 |
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