JPS6260101B2 - - Google Patents
Info
- Publication number
- JPS6260101B2 JPS6260101B2 JP9372079A JP9372079A JPS6260101B2 JP S6260101 B2 JPS6260101 B2 JP S6260101B2 JP 9372079 A JP9372079 A JP 9372079A JP 9372079 A JP9372079 A JP 9372079A JP S6260101 B2 JPS6260101 B2 JP S6260101B2
- Authority
- JP
- Japan
- Prior art keywords
- sheet
- water
- gel
- composition
- hydrogel
- 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
Links
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 22
- 239000000499 gel Substances 0.000 claims description 20
- 239000000463 material Substances 0.000 claims description 15
- 239000000017 hydrogel Substances 0.000 claims description 13
- 229910052782 aluminium Inorganic materials 0.000 claims description 4
- -1 aluminum compound Chemical class 0.000 claims description 4
- 229920001577 copolymer Polymers 0.000 claims description 4
- XJRBAMWJDBPFIM-UHFFFAOYSA-N methyl vinyl ether Chemical group COC=C XJRBAMWJDBPFIM-UHFFFAOYSA-N 0.000 claims description 4
- 150000003839 salts Chemical class 0.000 claims description 3
- 239000000203 mixture Substances 0.000 description 13
- 239000007864 aqueous solution Substances 0.000 description 4
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 238000010521 absorption reaction Methods 0.000 description 3
- 229940079593 drug Drugs 0.000 description 3
- 239000003814 drug Substances 0.000 description 3
- 238000001879 gelation Methods 0.000 description 3
- 230000014759 maintenance of location Effects 0.000 description 3
- 239000007900 aqueous suspension Substances 0.000 description 2
- 238000001816 cooling Methods 0.000 description 2
- JVTAAEKCZFNVCJ-UHFFFAOYSA-N lactic acid Chemical compound CC(O)C(O)=O JVTAAEKCZFNVCJ-UHFFFAOYSA-N 0.000 description 2
- 230000000717 retained effect Effects 0.000 description 2
- 239000005995 Aluminium silicate Substances 0.000 description 1
- 206010011985 Decubitus ulcer Diseases 0.000 description 1
- 239000004677 Nylon Substances 0.000 description 1
- 208000004210 Pressure Ulcer Diseases 0.000 description 1
- 206010037660 Pyrexia Diseases 0.000 description 1
- AZDRQVAHHNSJOQ-UHFFFAOYSA-N alumane Chemical class [AlH3] AZDRQVAHHNSJOQ-UHFFFAOYSA-N 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- WNROFYMDJYEPJX-UHFFFAOYSA-K aluminium hydroxide Chemical compound [OH-].[OH-].[OH-].[Al+3] WNROFYMDJYEPJX-UHFFFAOYSA-K 0.000 description 1
- 235000012211 aluminium silicate Nutrition 0.000 description 1
- 239000000440 bentonite Substances 0.000 description 1
- 229910000278 bentonite Inorganic materials 0.000 description 1
- SVPXDRXYRYOSEX-UHFFFAOYSA-N bentoquatam Chemical compound O.O=[Si]=O.O=[Al]O[Al]=O SVPXDRXYRYOSEX-UHFFFAOYSA-N 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 239000002537 cosmetic Substances 0.000 description 1
- 230000003111 delayed effect Effects 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 238000005538 encapsulation Methods 0.000 description 1
- 238000001704 evaporation Methods 0.000 description 1
- 230000008020 evaporation Effects 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- NLYAJNPCOHFWQQ-UHFFFAOYSA-N kaolin Chemical compound O.O.O=[Al]O[Si](=O)O[Si](=O)O[Al]=O NLYAJNPCOHFWQQ-UHFFFAOYSA-N 0.000 description 1
- 239000004310 lactic acid Substances 0.000 description 1
- 235000014655 lactic acid Nutrition 0.000 description 1
- 238000002386 leaching Methods 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 229920001778 nylon Polymers 0.000 description 1
- 230000035699 permeability Effects 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 229940126532 prescription medicine Drugs 0.000 description 1
- 235000011121 sodium hydroxide Nutrition 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000000725 suspension Substances 0.000 description 1
- 229920002994 synthetic fiber Polymers 0.000 description 1
- 239000012209 synthetic fiber Substances 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- 238000009834 vaporization Methods 0.000 description 1
- 230000008016 vaporization Effects 0.000 description 1
- 229920003169 water-soluble polymer Polymers 0.000 description 1
- 239000002759 woven fabric Substances 0.000 description 1
Classifications
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
- A61K8/00—Cosmetics or similar toiletry preparations
- A61K8/02—Cosmetics or similar toiletry preparations characterised by special physical form
- A61K8/04—Dispersions; Emulsions
- A61K8/042—Gels
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
- A61K8/00—Cosmetics or similar toiletry preparations
- A61K8/02—Cosmetics or similar toiletry preparations characterised by special physical form
- A61K8/0208—Tissues; Wipes; Patches
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
- A61K8/00—Cosmetics or similar toiletry preparations
- A61K8/18—Cosmetics or similar toiletry preparations characterised by the composition
- A61K8/72—Cosmetics or similar toiletry preparations characterised by the composition containing organic macromolecular compounds
- A61K8/81—Cosmetics or similar toiletry preparations characterised by the composition containing organic macromolecular compounds obtained by reactions involving only carbon-to-carbon unsaturated bonds
- A61K8/8164—Compositions of homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by a carboxyl radical, and containing at least one other carboxyl radical in the molecule, or of salts, anhydrides, esters, amides, imides or nitriles thereof; Compositions of derivatives of such polymers, e.g. poly (methyl vinyl ether-co-maleic anhydride)
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61Q—SPECIFIC USE OF COSMETICS OR SIMILAR TOILETRY PREPARATIONS
- A61Q19/00—Preparations for care of the skin
Landscapes
- Health & Medical Sciences (AREA)
- Life Sciences & Earth Sciences (AREA)
- Animal Behavior & Ethology (AREA)
- General Health & Medical Sciences (AREA)
- Public Health (AREA)
- Veterinary Medicine (AREA)
- Birds (AREA)
- Epidemiology (AREA)
- Dermatology (AREA)
- Chemical & Material Sciences (AREA)
- Dispersion Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Biomedical Technology (AREA)
- Medicinal Preparation (AREA)
- Cosmetics (AREA)
- Thermotherapy And Cooling Therapy Devices (AREA)
Description
【発明の詳細な説明】
この発明は、皮膚等に貼用して使用されるシー
ト状含水ゲルに関するものである。DETAILED DESCRIPTION OF THE INVENTION The present invention relates to a sheet-shaped hydrogel that is applied to the skin and the like.
メトキシエチレン・無水マレイン酸共重合体ま
たはその塩類の水溶液に、アルミニウム化合物の
水溶液または懸濁液を加え、PH3〜7の範囲で反
応させることによつて得られる含水ゲルは、つぎ
のような特性をもつている。 A hydrogel obtained by adding an aqueous solution or suspension of an aluminum compound to an aqueous solution of a methoxyethylene/maleic anhydride copolymer or its salts and reacting in a pH range of 3 to 7 has the following properties. It has
(1) 自己保形性
このゲルは、内部に多量の水を含むことがで
きるうえ、流動性が少く、強い弾力性を示し、
圧力を受けても容易に崩解しない。しかし張力
によつては容易に切断され、いわゆる展延性を
ほとんどもたない弾性ゲルである。(1) Self-shape retention This gel can contain a large amount of water inside, has low fluidity, and exhibits strong elasticity.
Does not disintegrate easily even under pressure. However, it is easily cut under tension and is an elastic gel with almost no malleability.
(2) 抱水性
内部にその容積の80%以上の水を含有させた
状態で圧縮しても水を吐き出すことがない。ま
たその表面に手を触れてもわずかに湿り気を感
ずるのみで、手を濡らすことはない。(2) Water-holding property Even if the material contains more than 80% of its volume of water and is compressed, no water will be expelled. Also, when you touch its surface, you only feel a slight dampness, and your hand does not get wet.
(3) 熱安定性
このゲルをアルミニウム箔の袋中に密封し
て、50℃の恒温槽中に2週間入れておいた後で
も原形も保持しており、蒸発によるもの以外に
はゲルの中からの、いわゆる離水現象の結果と
して生ずる水分の滲出は見られない。(3) Thermal stability Even after this gel was sealed in an aluminum foil bag and placed in a constant temperature bath at 50°C for two weeks, it retained its original shape, and the gel retained its original shape except for evaporation. No leaching of water as a result of the so-called syneresis phenomenon is observed.
(4) 透明性
ゲルの製造にあたつて、不溶性のアルミニウ
ム化合物の沈殿が系中に存在しないような条件
を選んで反応させた場合、得られたゲルは、き
わめて透明度が高く、均質である。(4) Transparency When producing a gel, if reaction conditions are selected such that no precipitation of insoluble aluminum compounds is present in the system, the resulting gel will be extremely transparent and homogeneous. .
(5) 吸水性
内部に多量の水を含んでいる状態でも、新ら
たに水と接触させると膨潤し、さらに大量の水
を吸収する。また水中にてゲルを投入すると、
体積で約3倍に膨張する。(5) Water absorption Even when it contains a large amount of water, it swells when it comes into contact with water and absorbs even more water. Also, if you put the gel in water,
Expands approximately 3 times in volume.
(6) 放湿性(吸熱性)
ゲルを室内に放置すると、表面から徐々に水
分を蒸発させる。このとき蒸発潜熱が奪われる
ため、ゲルは常に室温よりも低い温度に保たれ
る。(6) Moisture release (endotherm) When the gel is left indoors, water gradually evaporates from its surface. At this time, the latent heat of vaporization is taken away, so the gel is always kept at a temperature lower than room temperature.
この発明は、上記のような特性を有する含水ゲ
ルを、シツプ薬などの用途に容易に利用し得るよ
うにしたシート状含水ゲルを提供することを目的
としてなされたものである。すなわちこの発明の
シート状含水ゲルは、上記の高含水ゲル層中に、
透水性シート状物、たとえばシート状メツシユを
封入することによつて構成されたもので、張力に
弱く、しかも展延性に乏しいというゲルの欠点が
除去される。したがつてこのシート状含水ゲル
は、シツプ薬の基剤、発熱患部の冷却用品、床ず
れ防止用クツシヨン、パツク基剤、あるいは冷却
用鉢巻きのような医薬品、医療用具、化粧品、日
用品等の用途に有利に使用することができる。 The present invention has been made with the object of providing a sheet-shaped hydrogel having the above-mentioned characteristics, which can be easily used for applications such as prescription medicines. That is, the sheet-shaped hydrogel of the present invention has the above-mentioned high hydrogel layer,
It is constructed by enclosing a water-permeable sheet-like material, such as a sheet-like mesh, and eliminates the drawbacks of gel, such as being weak against tension and having poor spreadability. Therefore, this sheet-shaped hydrous gel can be used as a base for medicines, medical supplies, cosmetics, daily necessities, etc., as a base for medicines, cooling supplies for fever-affected areas, cushions and pack bases for preventing pressure sores, and cooling headbands. can be used to advantage.
これらの用途のために従来からゲル様のペース
トをシート状として使用するようにしたものは多
い。たとえばシツプ薬基剤の場合、ペースとはネ
ルなどの支持体の上に塗布または延展される。こ
のペーストは、天然または合成糊料、天然または
合成水溶性高分子化合物、天然または合成保水剤
および水を主体とする粘度の高い糊に、カオリ
ン、ベントナイト等の粉体成分を添加して得られ
る適度の粘弾性をもつた粘性ゾルからなり、塗布
または延展が可能で、支持体上で保形性を示し、
常温で流動性を示さない。しかしながら、長期保
存によつて、あるいは加熱、吸水によつて、品質
的な劣化を示すことは避けられない。 Many gel-like pastes have been used in sheet form for these purposes. For example, in the case of a drug base, the paste is applied or spread on a support such as flannel. This paste is obtained by adding powder components such as kaolin and bentonite to a highly viscous paste that is mainly composed of natural or synthetic thickeners, natural or synthetic water-soluble polymer compounds, natural or synthetic water-retaining agents, and water. It consists of a viscous sol with moderate viscoelasticity, can be applied or spread, shows shape retention on a support,
Does not show fluidity at room temperature. However, quality deterioration cannot be avoided due to long-term storage, heating, or water absorption.
これに対して、この発明で使用される高含水ゲ
ルは、自己保形性、抱水性、熱安定性、吸水性、
放湿性などの点で前記のようなすぐれた特性を有
する反面、シート状にするには粘性が不足し、張
力を受けたときに簡単に引きちぎれてしまい、ま
たシート状に成形し得たとしても、使用に際して
貼用場所における引張り、捻じれにより容易にち
ぎれてしまう欠点をもち、ネル等の支持体への塗
布、延展も困難である。 On the other hand, the high water content gel used in this invention has self-shape retention, water retention, thermal stability, water absorption,
Although it has the excellent properties mentioned above in terms of moisture dissipation, it does not have enough viscosity to be made into a sheet, and it easily tears when subjected to tension, and even if it can be formed into a sheet, it However, during use, it has the disadvantage that it easily tears due to tension or twisting at the place where it is applied, and it is also difficult to apply and spread it on a support such as flannel.
本発明者は、この高含水ゲルの長所をいかし、
その欠点である延展性の不足を補うべく研究を行
つた結果、高含水ゲル層中に透水性シート状物を
封入することで、この問題を解決することに成功
した。ゲル層中へのシート状物の封入は、皿状の
容器にゲル化していない状態の組成物を一定量だ
け流し込み、その上をシート状物で被覆し、この
シート状物をその自重で組成物中に、好ましくは
組成物の深さの半分まで沈下させ、この状態で組
成物をゲル化させることによつて行うことができ
る。このことから明らかなように、シート状物の
望ましい沈下を得るためには、組成物のゲル化速
度を制御することが必要であり、この制御は、メ
トキシエチレン・無水マレイン酸共重合体もしく
はその塩の水溶液に、アルミニウム化合物の水溶
液または懸濁液を加えた組成物のPH値を調節する
ことによつて行うことができる。PH3〜7の範囲
で制御する場合、PH値が高くなるにしたがつてゲ
ル化速度は遅くなり、PH4.5〜5.5の範囲では、ゲ
ル化時間は約4時間まで遅延させることが可能で
ある。 The present inventor took advantage of the advantages of this high water content gel,
As a result of conducting research to compensate for the lack of spreadability, we succeeded in solving this problem by encapsulating a water-permeable sheet material in a high water content gel layer. Encapsulation of a sheet-like material into a gel layer involves pouring a certain amount of the ungelled composition into a dish-shaped container, covering it with a sheet-like material, and allowing the sheet-like material to absorb the composition by its own weight. This can be carried out by submerging the composition into a substance, preferably to half the depth of the composition, and allowing the composition to gel in this state. As is clear from this, it is necessary to control the gelation rate of the composition in order to obtain the desired settling of the sheet-like material, and this control is achieved by using methoxyethylene/maleic anhydride copolymer or its gelling rate. This can be done by adjusting the PH value of a composition in which an aqueous solution or suspension of an aluminum compound is added to an aqueous solution of a salt. When controlling in the PH range of 3 to 7, the higher the PH value, the slower the gelation rate becomes, and in the PH range of 4.5 to 5.5, the gelation time can be delayed up to about 4 hours. .
また皿状の容器内にその深さの約半分まで組成
物を流し込み、これをゲル化させたのちその上に
シート状をおき、この上から組成物を流し込んで
ゲル化させることによつても、シート状物を含水
ゲル層中に封入することができる。なお、シート
状物は含水ゲル層中に完全に封入されることが好
ましいが、シート状物の一部が含水ゲル層の表面
に露出していても差支えない。 It is also possible to pour the composition into a dish-shaped container to about half its depth, allow it to gel, place a sheet on top of it, and pour the composition from above to gel it. , a sheet-like material can be encapsulated in a hydrogel layer. Although it is preferable that the sheet-like material be completely encapsulated in the hydrogel layer, there is no problem even if a part of the sheet-like material is exposed on the surface of the hydrogel layer.
この発明で使用される透水性シート状物とは、
ゲル化していない組成物が滲出または通過できる
ような透水性を有するシート状物で、不透水性シ
ート状物に透孔を設けたものでもよいが、とくに
シート状のメツシユ体が好ましい。このようなシ
ート状メツシユ体としては、ガーゼ、寒冷紗、荒
目の織布または不織布、ナイロンネツト、荒目の
天然または合成繊維層などをあげることができ
る。ただし水に不溶のものでなければならない。
また封入は1シートに限らず、複数シートを、た
とえばスクランブルに封入してもよい。 The water permeable sheet material used in this invention is:
A sheet-like material having water permeability that allows the non-gelled composition to exude or pass through, and a water-impermeable sheet material having through holes provided therein, may also be used, but a sheet-like mesh material is particularly preferred. Examples of such sheet-like mesh bodies include gauze, cheesecloth, coarse woven or nonwoven fabrics, nylon nets, coarse natural or synthetic fiber layers, and the like. However, it must be insoluble in water.
Moreover, the enclosure is not limited to one sheet, but a plurality of sheets may be enclosed, for example, in a scrambled manner.
つぎにこの発明の実施例について説明する。 Next, embodiments of the invention will be described.
水500ml中に、メトキシエチレン・無水マレイ
ン酸共重合体50gを溶かす。これに苛性ソーダ17
gおよび2M乳酸100mlを加えてPHを4.5〜5に調
整し、さらに2.5%水酸化アルミニウム懸濁液190
mlを加え、つぎに水を加えて全量を1000gとす
る。ここに得られた組成物を第1図に示す皿状の
容器1内に所望の深さになるまで流し込み、その
表面にシート状メツシユ2をのせた。このシート
状メツシユ2は、その自重で徐々に沈下し、数分
後に組成物の深さの約半分まで沈下した。組成物
は約1時間後に流動性を失い、その後に表面を薄
紙4で被覆した。 Dissolve 50 g of methoxyethylene/maleic anhydride copolymer in 500 ml of water. Caustic soda 17 to this
Add g and 100 ml of 2M lactic acid to adjust the pH to 4.5-5, and then add 2.5% aluminum hydroxide suspension 190
ml, then add water to make a total volume of 1000g. The composition obtained here was poured into a dish-shaped container 1 shown in FIG. 1 to a desired depth, and a sheet-shaped mesh 2 was placed on the surface thereof. This sheet-like mesh 2 gradually sank due to its own weight, and after several minutes sank to about half the depth of the composition. The composition lost its fluidity after about 1 hour, after which the surface was covered with tissue paper 4.
得られたシート状含水ゲルは、第2図に示すよ
うに、ゲル3のほぼ中央部にシート状メツシユ2
が封入されたもので、その表面は薄紙4で被覆さ
れている。 The obtained sheet-shaped hydrogel has a sheet-shaped mesh 2 approximately in the center of the gel 3, as shown in FIG.
is enclosed, and its surface is covered with thin paper 4.
第1図はこの発明の一実施例によつて得られた
シート状含水ゲルを示す縦断面図、第2図は同シ
ート状含水ゲルの一部切欠斜視図である。
1……容器、2……シート状メツシユ、3……
含水ゲル、4……薄紙。
FIG. 1 is a longitudinal sectional view showing a sheet-shaped hydrogel obtained according to an embodiment of the present invention, and FIG. 2 is a partially cutaway perspective view of the same sheet-shaped hydrogel. 1... Container, 2... Sheet mesh, 3...
Hydrogel, 4...Thin paper.
Claims (1)
もしくはその塩類と、アルミニウム化合物とを主
体としたシート状の高含水ゲル層中に、透水性シ
ート状物を封入してなるシート状含水ゲル。1. A sheet-like hydrogel formed by enclosing a water-permeable sheet-like material in a sheet-like high-water-containing gel layer mainly composed of a methoxyethylene/maleic anhydride copolymer or its salts and an aluminum compound.
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
JP9372079A JPS5618917A (en) | 1979-07-25 | 1979-07-25 | Sheet hydrous gel |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
JP9372079A JPS5618917A (en) | 1979-07-25 | 1979-07-25 | Sheet hydrous gel |
Publications (2)
Publication Number | Publication Date |
---|---|
JPS5618917A JPS5618917A (en) | 1981-02-23 |
JPS6260101B2 true JPS6260101B2 (en) | 1987-12-15 |
Family
ID=14090241
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
JP9372079A Granted JPS5618917A (en) | 1979-07-25 | 1979-07-25 | Sheet hydrous gel |
Country Status (1)
Country | Link |
---|---|
JP (1) | JPS5618917A (en) |
Families Citing this family (10)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JPS58209519A (en) * | 1982-05-31 | 1983-12-06 | Toray Ind Inc | Water-containing gel for casting with buried substance having arbitrary configuration |
JPS59181208A (en) * | 1983-03-31 | 1984-10-15 | Horiuchi Itarou Shoten:Kk | Drug for external use |
US4600078A (en) * | 1983-12-12 | 1986-07-15 | Lockheed Corporation | Sound barrier |
JPS60190712A (en) * | 1984-03-12 | 1985-09-28 | Daikyo Yakuhin Kogyo Kk | Poultice usable also as bandage |
US4769022A (en) * | 1986-05-02 | 1988-09-06 | Minnesota Mining And Manufacturing Company | Cleansing pad |
JPS642647A (en) * | 1987-06-25 | 1989-01-06 | Tatsuya Kano | Wet compress article |
US4891313A (en) * | 1988-01-21 | 1990-01-02 | Boehringer Manheim Corporation | Method for determination of a component of a sample |
US5115801A (en) * | 1990-05-02 | 1992-05-26 | Ndm Acquisition Corp. | Hydrogel burn dressing product |
US5154706A (en) * | 1991-08-07 | 1992-10-13 | Ndm Acquisition Corp. | Wound dressing for deep wounds |
DE69930869T2 (en) * | 1998-12-03 | 2006-11-30 | Kao Corp. | COSMETIC LAYER |
-
1979
- 1979-07-25 JP JP9372079A patent/JPS5618917A/en active Granted
Also Published As
Publication number | Publication date |
---|---|
JPS5618917A (en) | 1981-02-23 |
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