JPH0339729B2 - - Google Patents
Info
- Publication number
- JPH0339729B2 JPH0339729B2 JP60069531A JP6953185A JPH0339729B2 JP H0339729 B2 JPH0339729 B2 JP H0339729B2 JP 60069531 A JP60069531 A JP 60069531A JP 6953185 A JP6953185 A JP 6953185A JP H0339729 B2 JPH0339729 B2 JP H0339729B2
- Authority
- JP
- Japan
- Prior art keywords
- adsorbent
- narrow
- filled
- carbon dioxide
- amine
- 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
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/02—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2253/00—Adsorbents used in seperation treatment of gases and vapours
- B01D2253/25—Coated, impregnated or composite adsorbents
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2253/00—Adsorbents used in seperation treatment of gases and vapours
- B01D2253/30—Physical properties of adsorbents
- B01D2253/34—Specific shapes
- B01D2253/342—Monoliths
- B01D2253/3425—Honeycomb shape
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/50—Carbon oxides
- B01D2257/504—Carbon dioxide
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
- Y02C20/00—Capture or disposal of greenhouse gases
- Y02C20/40—Capture or disposal of greenhouse gases of CO2
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Analytical Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Treating Waste Gases (AREA)
Description
〔産業上の利用分野〕
本発明は、多孔質表面を有する粒状固体表面に
炭酸ガスと親和性のあるアミン系有機物質を付着
させた固体吸着材を用い、吸着材のCO2吸収力を
最大限に発揮し得る充てん層セル構造を備えた炭
酸ガス除去装置、詳しくは、比表面積のきわめて
大なる粒状固体吸着材と被処理ガスとの接触時間
を向上させ、さらに広い内表面を有する充てんセ
ル構造体内面にも、CO2吸収力を持たせることに
より、効率良くCO2を除去することができる炭酸
ガス除去装置に関するものである。
〔従来の技術〕
従来、炭酸ガス除去装置として、CO2と親和力
のあるポリエチレンイミン、テトラエチレンアミ
ンペンタンなどを、比表面積のきわめて大なる多
孔質粒状固体表面に付着させた吸着材を用いる研
究例が知られている。
〔発明が解決しようとする課題〕
この場合、比表面積が大きなものを用いるため
に、必然的に粒子径は１mm以下の小さなものにな
り、充てん構造体に詰めてガスを流通する時、ガ
スの通気抵抗が大きい上、ガス流が偏流を起こす
ことによつて、すべての固体吸着材にCO2が吸着
されることがなく、充てん吸着材のCO2吸着力を
完全に得ることができないという問題点がある。
本発明者らは、この従来技術の問題点を解決す
るために鋭意研究を行い、種々検討を重ねた結
果、ガスの偏流をなくしすべての充てん吸着材が
均一に、しかも、ほぼ完全にCO2を飽和吸着でき
る方法を見い出した。すなわち、ガス流に直角方
向の断面形状が、粒状吸着材の平均直径の２〜10
倍の平均内径を有する格子状、ハニカム状、波形
状のような多数の狭流路を備えたセル構造体の内
部に、吸着材を単純充てんすることによつて、吸
着材と吸着材、および吸着材と壁面がブリツジを
形成するようになり、ガスの通過しやすい狭流路
をランダムに形成することになる。
ここで形成される狭流路は、通気抵抗が小さい
にもかかわらず複雑であるため、固体吸着材とガ
スとの接触が飛躍的に向上し、吸着材のCO2吸収
力を十分に発揮させることができる。さらに、格
子状、ハニカム状、波形状などに並ぶ狭流路壁面
を構成する材料にも、アミン系有機物質を付着さ
せた多孔質材を用いることによつて、さらに容積
当りのCO2吸収力を増加させることができる。
本発明は、上記の知見に基づきなされたもの
で、潜水艦、宇宙船のように外部環境とほとんど
隔絶された密閉空間内における、人間、その他動
物の排出するCO2ガスを乾式で吸着除去する装置
として、充てん構造体の構造を工夫し、かつ新規
な方式を採用することによつて、吸着力のきわめ
て大なる炭酸ガス除去装置を提供することを目的
とするものである。
また、本発明は、炭酸ガス除去装置の炭酸ガス
吸着材として、多孔質粒状固体の表面にアミン系
有機物を付着させたものに着目し、そのCO2吸収
力を飛躍的に向上させるようにした炭酸ガス除去
装置を提供することを目的とするものである。
〔課題を解決するための手段および作用〕
上記の目的を達成するために、本願の第１の発
明の炭酸ガス除去装置は、外部環境とほとんど隔
絶した密閉空間内における、人間等の排出する
CO2ガスを乾式で吸着除去する装置であつて、
多孔質材の表面にアミン系有機物質を付着させ
た粒状固体を吸着材とし、
この固体吸着材の平均粒径の２〜10倍の平均内
径を有する多数の狭流路を備えたセル構造体の各
狭流路内に、前記吸着材を充てんしたことを特徴
としている。
また、本願の第２の発明の炭酸ガス除去装置
は、外部環境とほとんど隔絶した密閉空間内にお
ける、人間等の排出するCO2ガスを乾式で吸着除
去する装置であつて、
多孔質材の表面にアミン系有機物質を付着させ
た粒状固体を吸着材とし、
この固体吸着材の平均粒径の２〜10倍の平均内
径を有する多数の狭流路を備えたセル構造体の各
狭流路内に、前記吸着材を充てんし、
セル構造体の各狭流路の内表面にアミン系有機
物質を付着させたことを特徴としている。
なお、狭流路の平均内径が、粒状固体吸着剤の
平均粒径の２倍未満の場合は、充てん効率が低下
するために、全体として容積当りの吸着能力は低
下することとなる。２倍未満の狭流路における充
てん効率低下の要因は、壁面とのブリツジ効果に
よるものであり、文献等にも示されている（例え
ば、R.W.Schuler、et al；CEP.Symposium
Ser.、48、No.4.19（1952））。一方、狭流路の平均
内径が、粒状固体吸着剤の平均粒径の10倍を超え
る場合は、吸着時に発生する吸着熱の伝導による
冷却効果が悪くなるため、事実上、全体としての
吸着能力が低下し、使用に耐えないものとなる。
なお、10倍という数字は、本発明の具体的使用目
的である生命維持装置のCO2吸着剤として、特許
請求の範囲の吸着剤を使用する場合における吸着
性能に起因する。
以下、図面に基づいて説明する。
第１図は、本発明の粒状固体吸着材を用いた
CO2除去装置の基本フローを示したものである。
そのシステムは密閉空間内の呼吸気ガスをフアン
１によつて固体吸着材を充てんした充てん層２に
吸引し、内部の固体吸着材３によつてCO2を吸着
せしめ、切換弁４を介して、望ましくはフイルタ
ー６を介して再び密閉空間へ処理済みエアとして
戻す方式である。ここでもう１つの充てん層７は
充てん層２と同じ構造で、内部に固体吸着材を充
てんしたものである。ここでは、既にCO2を吸着
し終つた吸着材を加熱、あるいは減圧吸引によつ
てCO2を分離脱着し、空間内エア循環流路とは異
なる流路８を通して、空間の外部へ排出あるいは
蓄積するシステムとなつている。この操作によつ
て、充てん層７は再びCO2吸着力を回復し、充て
ん層２がCO2吸着力を失つた時点で、弁４を切り
換えることによりCO2の吸着を開始する。この複
数個の充てん層を有する第１図のCO2除去装置
は、空間内エアの浄化とCO2の除去とを、同時
に、かつ連続的に行うことができる。５，８はラ
イン、１０はコンプレツサー、１１はCO2タン
ク、１２は加熱・冷却ライン、１３はCO2ライ
ン、１４，１５は切換弁である。
本発明の炭酸ガス除去装置とは、第１図の充て
ん層２および充てん層７の内部構造に関するもの
である。
〔実施例〕
以下、実施例を上げて本発明をさらに具体的に
説明するが、本発明はこれらの実施例によつて限
定されるものではなく、種々の応用実施が可能で
ある。
実施例 １
第２図〜第４図は、充てん層を形成するのに用
いた格子１６を有する格子状セル構造体１７であ
り、材料は多孔質でポリエチレンイミンを付着さ
せたアルミナでできている。なお、格子１６の内
径Ｄは3.0mmである。
第２図に示すセル構造体に、0.5〜1.0mmの平均
径を有する多孔質アクリル樹脂でできたポリエチ
レンイミンを付着させた粒状固体吸着材３を単純
充てんした時、第１表の実験結果に示すように、
同一固体吸着材を狭流路のない構造体に充てんし
た場合と比べ、約1.3倍CO2吸収力が増加した。
なお、第４図は、狭流路をガス流れ方向に切断し
た図であり、吸着剤３の充てん状態を示してい
る。
[Industrial Application Field] The present invention uses a solid adsorbent in which an amine-based organic substance that has an affinity for carbon dioxide gas is attached to the surface of a granular solid having a porous surface, and maximizes the CO 2 absorption capacity of the adsorbent. A carbon dioxide removal device equipped with a packed layer cell structure that can achieve maximum performance, specifically, a packed cell that improves the contact time between a granular solid adsorbent with an extremely large specific surface area and the gas to be treated, and has a wider inner surface. This invention relates to a carbon dioxide removal device that can efficiently remove CO 2 by providing CO 2 absorption capacity to the inner surface of the structure. [Conventional technology] Conventionally, as a carbon dioxide removal device, an example of research using an adsorbent in which polyethyleneimine, tetraethyleneamine pentane, etc., which have an affinity for CO 2 , is attached to the surface of a porous granular solid with an extremely large specific surface area. It has been known. [Problem to be solved by the invention] In this case, since particles with a large specific surface area are used, the particle size inevitably becomes small, 1 mm or less, and when the gas is passed through the filling structure, the gas is In addition to high ventilation resistance, due to uneven gas flow, CO 2 is not adsorbed by all solid adsorbents, and the full CO 2 adsorption power of the filled adsorbent cannot be obtained. There is a point. The inventors of the present invention have conducted extensive research to solve the problems of the conventional technology, and as a result of various studies, they have found that by eliminating the uneven flow of gas, all the filled adsorbents are uniformly distributed, and moreover, CO 2 is almost completely removed. We have discovered a method that allows for saturated adsorption of In other words, the cross-sectional shape perpendicular to the gas flow is 2 to 10 times the average diameter of the granular adsorbent.
By simply filling the adsorbent inside a cell structure with a large number of narrow channels such as a lattice-like, honeycomb-like, or wave-like structure having twice the average inner diameter, the adsorbent, the adsorbent, and The adsorbent and the wall surface form bridges, randomly forming narrow channels through which gas can easily pass. The narrow flow path formed here is complex despite having low ventilation resistance, which dramatically improves the contact between the solid adsorbent and the gas, allowing the adsorbent to fully utilize its CO 2 absorption capacity. be able to. Furthermore, by using porous materials to which amine-based organic substances are attached for the materials that make up the walls of the narrow channels arranged in a lattice, honeycomb, or wave shape, we can further increase the CO 2 absorption capacity per volume. can be increased. The present invention was made based on the above knowledge, and is a device for dry adsorption and removal of CO 2 gas emitted by humans and other animals in a closed space that is almost isolated from the outside environment, such as a submarine or spacecraft. The purpose of this invention is to provide a carbon dioxide removal device with extremely high adsorption power by devising the structure of the filling structure and adopting a new method. Furthermore, the present invention focuses on a material in which amine-based organic matter is attached to the surface of a porous granular solid as a carbon dioxide adsorbent for a carbon dioxide removal device, and dramatically improves its CO 2 absorption capacity. The purpose of this invention is to provide a carbon dioxide removal device. [Means and operations for solving the problem] In order to achieve the above object, the carbon dioxide removal device of the first invention of the present application is designed to remove the carbon dioxide gas from a person or the like in a closed space that is almost isolated from the outside environment.
This is a device that dry-adsorbs and removes CO 2 gas, and uses a granular solid with an amine-based organic substance attached to the surface of a porous material as an adsorbent. The present invention is characterized in that the adsorbent is filled in each narrow channel of a cell structure having a large number of narrow channels each having an inner diameter. Further, the carbon dioxide removal device of the second invention of the present application is a device that dry-adsorbs and removes CO 2 gas emitted by humans etc. in a closed space that is almost isolated from the external environment, and which The adsorbent is a granular solid to which an amine-based organic substance is attached, and each narrow channel of the cell structure is equipped with a large number of narrow channels having an average inner diameter of 2 to 10 times the average particle diameter of the solid adsorbent. The cell structure is characterized in that the adsorbent is filled inside the cell structure, and an amine-based organic substance is attached to the inner surface of each narrow channel of the cell structure. Note that if the average inner diameter of the narrow flow path is less than twice the average particle diameter of the granular solid adsorbent, the filling efficiency will decrease, resulting in a decrease in the adsorption capacity per volume as a whole. The reason for the decrease in filling efficiency in a narrow flow path of less than 2 times is due to the bridge effect with the wall surface, which is also shown in the literature (for example, RWSchuler, et al; CEP.Symposium
Ser., 48, No. 4.19 (1952)). On the other hand, if the average inner diameter of the narrow channel exceeds 10 times the average particle diameter of the granular solid adsorbent, the cooling effect due to the conduction of the adsorption heat generated during adsorption will deteriorate, and the overall adsorption capacity will actually decrease. decreases and becomes unusable.
Note that the number 10 times is due to the adsorption performance when the adsorbent of the claims is used as a CO 2 adsorbent for a life support device, which is a specific purpose of use of the present invention. The description will be given below based on the drawings. Figure 1 shows a sample using the granular solid adsorbent of the present invention.
This shows the basic flow of the CO 2 removal device.
The system uses a fan 1 to suck respiratory gas in a closed space into a packed layer 2 filled with a solid adsorbent, and a solid adsorbent 3 inside adsorbs CO2 , which is then passed through a switching valve 4. It is preferable to return the treated air to the closed space via a filter 6 as treated air. Here, the other filled layer 7 has the same structure as the filled layer 2, and is filled with a solid adsorbent. Here, CO 2 is separated and desorbed by heating the adsorbent that has already adsorbed CO 2 or by vacuum suction, and then discharged or accumulated outside the space through a flow path 8 different from the air circulation flow path within the space. The system is designed to do this. By this operation, the packed layer 7 regains its CO 2 adsorption ability, and when the filled layer 2 loses its CO 2 adsorption ability, it starts adsorbing CO 2 by switching the valve 4. The CO 2 removal device shown in FIG. 1 having a plurality of filling layers can purify the air in the space and remove CO 2 simultaneously and continuously. 5 and 8 are lines, 10 is a compressor, 11 is a CO 2 tank, 12 is a heating/cooling line, 13 is a CO 2 line, and 14 and 15 are switching valves. The carbon dioxide removal device of the present invention relates to the internal structure of the filled layer 2 and the filled layer 7 shown in FIG. [Examples] Hereinafter, the present invention will be explained in more detail with reference to Examples, but the present invention is not limited to these Examples, and various applications are possible. Example 1 Figures 2 to 4 show a lattice-like cell structure 17 having a lattice 16 used to form a filling layer, and the material is porous and made of alumina to which polyethyleneimine is attached. . Note that the inner diameter D of the grating 16 is 3.0 mm. When the cell structure shown in Fig. 2 was simply filled with granular solid adsorbent 3 made of porous acrylic resin with an average diameter of 0.5 to 1.0 mm and attached with polyethyleneimine, the experimental results shown in Table 1 were obtained. As shown,
Compared to a structure without narrow channels filled with the same solid adsorbent, the CO 2 absorption capacity increased approximately 1.3 times.
In addition, FIG. 4 is a diagram in which the narrow flow path is cut in the gas flow direction, and shows the state in which the adsorbent 3 is filled.
【表】【table】
本発明の炭酸ガス除去装置は上記のように構成
されているので、潜水艦、宇宙船等のみならず、
密閉空間内の環境制御装置において、CO2を効率
よく、かつ安定して吸着除去することができると
いう効果を奏する。
Since the carbon dioxide removal device of the present invention is configured as described above, it can be used not only for submarines, spaceships, etc.
In an environment control device in a closed space, CO 2 can be efficiently and stably adsorbed and removed.
第１図は本発明の装置の一例を示すフローシー
ト、第２図は本発明の実施例に用いた充てんセル
構造体の斜視図、第３図はその一部拡大図、第４
図は開孔（狭流路）内の吸着剤の充てん状態を示
す説明図、第５図〜第７図はセル構造体の他の実
施例を示す説明図である。
１……フアン、２，７……充てん層、３……吸
着材、４……切換弁、５……ライン、６……フイ
ルター、８……ライン、１０……コンプレツサ
ー、１１……CO2タンク、１２……加熱・冷却ラ
イン、１３……CO2ライン、１４，１５……切換
弁、１６……格子、１７……格子状セル構造体、
１８，１９，２０……開孔（狭流路）。
FIG. 1 is a flow sheet showing an example of the apparatus of the present invention, FIG. 2 is a perspective view of a filled cell structure used in an embodiment of the present invention, FIG. 3 is a partially enlarged view thereof, and FIG.
The figure is an explanatory view showing the filling state of the adsorbent in the opening (narrow flow path), and FIGS. 5 to 7 are explanatory views showing other embodiments of the cell structure. 1...Fan, 2,7...Filled layer, 3...Adsorbent, 4...Switching valve, 5...Line, 6...Filter, 8...Line, 10...Compressor, 11...CO 2 tank, 12... heating/cooling line, 13... CO 2 line, 14, 15... switching valve, 16... lattice, 17... lattice cell structure,
18, 19, 20...Open hole (narrow flow path).
Claims (1)
ける、人間等の排出するCO2ガスを乾式で吸着除
去する装置であつて、 多孔質材の表面にアミン系有機物質を付着させ
た粒状固体を吸着材とし、 この固体吸着材の平均粒径の２〜10倍の平均内
径を有する多数の狭流路を備えたセル構造体の各
狭流路内に、前記吸着材を充てんしたことを特徴
とする炭酸ガス除去装置。 ２ 外部環境とほとんど隔絶した密閉空間内にお
ける、人間等の排出するCO2ガスを乾式で吸着除
去する装置であつて、 多孔質材の表面にアミン系有機物質を付着させ
た粒状固体を吸着材とし、 この固体吸着材の平均粒径の２〜10倍の平均内
径を有する多数の狭流路を備えたセル構造体の各
狭流路内に、前記吸着材を充てんし、 セル構造体の各狭流路の内表面にアミン系有機
物質を付着させたことを特徴とする炭酸ガス除去
装置。[Scope of Claims] 1. A device for dry adsorption and removal of CO 2 gas emitted by humans, etc. in a closed space almost isolated from the outside environment, comprising an amine-based organic substance attached to the surface of a porous material. The adsorbent is filled in each narrow channel of a cell structure comprising a large number of narrow channels having an average inner diameter 2 to 10 times the average particle diameter of the solid adsorbent. A carbon dioxide removal device characterized by: 2 A device that dry-adsorbs and removes CO 2 gas emitted by humans in a closed space that is almost isolated from the outside environment, and uses granular solids with amine-based organic substances attached to the surface of a porous material as an adsorbent. The adsorbent is filled in each narrow passage of a cell structure having a large number of narrow passages each having an average inner diameter of 2 to 10 times the average particle diameter of the solid adsorbent. A carbon dioxide removal device characterized in that an amine-based organic substance is attached to the inner surface of each narrow flow path.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP60069531A JPS61227822A (en) | 1985-04-01 | 1985-04-01 | Removing device for carbonic acid gas |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP60069531A JPS61227822A (en) | 1985-04-01 | 1985-04-01 | Removing device for carbonic acid gas |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS61227822A JPS61227822A (en) | 1986-10-09 |
| JPH0339729B2 true JPH0339729B2 (en) | 1991-06-14 |
Family
ID=13405396
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP60069531A Granted JPS61227822A (en) | 1985-04-01 | 1985-04-01 | Removing device for carbonic acid gas |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS61227822A (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2005082489A1 (en) | 2004-02-27 | 2005-09-09 | Shimadzu Corporation | Apparatus and tool for adsorbing carbon dioxide and method for manufacture thereof |
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| JP4772852B2 (en) * | 2008-11-20 | 2011-09-14 | 川崎重工業株式会社 | Heat resistant carbon dioxide absorbent, production method thereof, carbon dioxide absorption method and carbon dioxide absorption apparatus using the same |
| JP2014511272A (en) * | 2011-02-28 | 2014-05-15 | コーニング インコーポレイテッド | Articles for capturing carbon dioxide |
| US20130207034A1 (en) * | 2012-02-09 | 2013-08-15 | Corning Incorporated | Substrates for carbon dioxide capture and methods for making same |
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| US11083989B2 (en) | 2014-06-04 | 2021-08-10 | Haldor Topsøe A/S | Gas treatment monolith article |
| CN106659962B (en) | 2014-08-20 | 2019-06-21 | 夏普株式会社 | Carbon dioxide concentration control system and carbon dioxide concentration control device |
| WO2019161114A1 (en) | 2018-02-16 | 2019-08-22 | Carbon Sink, Inc. | Fluidized bed extractors for capture of co2 from ambient air |
| JP7712776B2 (en) * | 2021-03-10 | 2025-07-24 | イビデン株式会社 | Carbon dioxide capture system and carbon dioxide capture method |
| WO2025183170A1 (en) * | 2024-03-01 | 2025-09-04 | ダイキン工業株式会社 | Adsorption device and adsorption system |
-
1985
- 1985-04-01 JP JP60069531A patent/JPS61227822A/en active Granted
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2005082489A1 (en) | 2004-02-27 | 2005-09-09 | Shimadzu Corporation | Apparatus and tool for adsorbing carbon dioxide and method for manufacture thereof |
Also Published As
| Publication number | Publication date |
|---|---|
| JPS61227822A (en) | 1986-10-09 |
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