JP2583151B2 - Method for producing deodorant composite material - Google Patents
Method for producing deodorant composite materialInfo
- Publication number
- JP2583151B2 JP2583151B2 JP2222202A JP22220290A JP2583151B2 JP 2583151 B2 JP2583151 B2 JP 2583151B2 JP 2222202 A JP2222202 A JP 2222202A JP 22220290 A JP22220290 A JP 22220290A JP 2583151 B2 JP2583151 B2 JP 2583151B2
- Authority
- JP
- Japan
- Prior art keywords
- adsorbent
- sulfate
- composite material
- porous substrate
- present
- 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
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- Disinfection, Sterilisation Or Deodorisation Of Air (AREA)
- Treating Waste Gases (AREA)
- Separation Of Gases By Adsorption (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Description
【発明の詳細な説明】 (産業上の利用分野) 本発明は、脱臭性複合材料の製造方法に関する。Description: TECHNICAL FIELD The present invention relates to a method for producing a deodorizable composite material.
(従来の技術) 従来、気体又は液体中の臭気やその他の微量成分を除
去するために、吸着剤を各種多孔性基材に固定した吸着
材料が用いられている。(Prior Art) Conventionally, an adsorbent material in which an adsorbent is fixed to various porous substrates has been used to remove odors and other trace components in a gas or liquid.
このような吸着材料については各種提案されている。
その代表的なものとしては、吸着剤を高分子エマルジョ
ンや水溶性高分子等の各種バインダー成分に分散させた
ものを、多孔性基材に含浸又は塗布して付着させた吸着
材料がある。また、この吸着材料においては、バインダ
ーが吸着剤の表面をかなり被覆してしまって吸着性能が
発揮されないことがあるため、あらかじめ多孔性基材に
バインダーを塗布した後、吸着剤を固着することによる
改良が提案されている。Various proposals have been made for such adsorption materials.
As a typical example, there is an adsorbent material in which an adsorbent is dispersed in various binder components such as a polymer emulsion or a water-soluble polymer and impregnated or applied to a porous base material. Also, in this adsorbent material, since the binder may cover the surface of the adsorbent considerably and the adsorbing performance may not be exhibited, it is necessary to apply the binder to the porous substrate in advance and fix the adsorbent. Improvements have been proposed.
(発明が解決しようとする課題) しかしながら、この改良された吸着材料では多孔性基
材と吸着剤とが、ごく一部で接着されているだけである
ため、吸着剤の脱落が避けられない。これを防ぐため
に、吸着剤の表層に更にバインダーを塗布することが推
奨されている。これにより、ある程度表層の吸着剤の脱
落は防げるものの、多孔性基材内部の吸着剤の脱落は防
げないし、吸着能力の低下も起こるという問題が生じ
る。(Problems to be Solved by the Invention) However, in the improved adsorbent material, the porous substrate and the adsorbent are only partially adhered to each other, so that the adsorbent is inevitably dropped. In order to prevent this, it is recommended to further apply a binder to the surface layer of the adsorbent. As a result, the adsorbent on the surface layer can be prevented from falling off to some extent, but the adsorbent inside the porous substrate cannot be dropped off, and the adsorbing ability is reduced.
また特開昭59−48242等には、陽イオン無機繊維、活
性炭及びアニオン性バインダーを含有するスラリーから
湿式抄紙法で吸着性シートを製造する方法が開示されて
いる。しかしながら、この方法は、アスベスト繊維等を
使用するため、衛生上の問題がある。JP-A-59-48242 discloses a method for producing an adsorptive sheet from a slurry containing cationic inorganic fibers, activated carbon and an anionic binder by a wet papermaking method. However, this method has a hygienic problem because it uses asbestos fiber and the like.
本発明者らは上記のような欠点のない吸着材料を得る
べく鋭意努力した結果、多孔性基材と吸着剤とをバイン
ダーで接着固定せしめ、更にその表面を特定の化合物で
処理すれば、吸着剤の脱落を防ぐことができ、加えて脱
臭性能も向上することを見出し、この知見に基き更に検
討を進めた結果、本発明を完成するに至った。The present inventors have worked diligently to obtain an adsorbent material free from the above-mentioned drawbacks. As a result, the porous substrate and the adsorbent are bonded and fixed with a binder, and the surface is treated with a specific compound. The present inventors have found that the agent can be prevented from falling off, and that the deodorizing performance is also improved, and further studies based on this finding have led to the completion of the present invention.
(課題を解決するための手段) かくして本発明によれば、多孔性基材にバインダーで
吸着剤を接着固定し、次いで硫酸アルミニウム及び遷移
金属の硫酸塩を含有させることを特徴とする脱臭性複合
材料の製造方法が提供される。(Means for Solving the Problems) Thus, according to the present invention, an adsorbent is fixedly adhered to a porous substrate with a binder, and then aluminum sulfate and a sulfate of a transition metal are contained. A method of manufacturing a material is provided.
本発明において用いる多孔性基材は、空隙率が0.3%
以上の多孔性物質である。その具体例としては、発泡樹
脂、不織布、紙、布等が挙げられるが、なかでもポリウ
レタンフォームや不織布が好ましい。これらの多孔性物
質の孔の径、形状等に制限はない。The porous substrate used in the present invention has a porosity of 0.3%
The above is a porous substance. Specific examples thereof include foamed resin, non-woven fabric, paper, cloth and the like, and among them, polyurethane foam and non-woven fabric are preferable. There is no limitation on the diameter, shape, etc. of the pores of these porous substances.
本発明において用いる吸着剤は、比表面積が50m2/g以
上、好ましくは100m2/g以上のものであればよく、その
具体例としては、活性炭、シリカゲル、アルミナ、ゼオ
ライト、クレー、ベントナイト、ケイソウ土、酸性白土
等が挙げられる。なかでも活性炭が好ましい。活性炭の
形状は粉末炭、粒状炭のいずれでもよく、原料は植物系
の木材、ヤシ殻や鉱物系の石炭、石油残さ等のいずれで
もよい。The adsorbent used in the present invention has a specific surface area of 50 m 2 / g or more, preferably 100 m 2 / g or more, and specific examples thereof include activated carbon, silica gel, alumina, zeolite, clay, bentonite, and diatomaceous earth. Soil, acid clay, and the like. Among them, activated carbon is preferred. The shape of the activated carbon may be any of powdered charcoal and granular charcoal, and the raw material may be any of plant-based wood, coconut shell, mineral-based coal, petroleum residue, and the like.
本発明の脱臭性複合材料の製造方法において、多孔性
基材と吸着剤との重量比は、通常、1:10〜100:1であ
る。吸着剤がこの範囲を外れて少ないときは、脱臭性能
が劣り、逆にこの範囲を外れて多いときは、多孔性基材
との接着固定が不十分となる部分が生じる。In the method for producing a deodorizable composite material of the present invention, the weight ratio between the porous substrate and the adsorbent is usually from 1:10 to 100: 1. When the amount of the adsorbent is small outside this range, the deodorizing performance is inferior. On the other hand, when the amount is outside this range, there are portions where the adhesive fixation to the porous substrate is insufficient.
本発明において用いるバインダーは、特に限定されな
い。具体例としては、合成樹脂エマルジョン接着剤、ゴ
ムラテックス接着剤、各種ゴムや樹脂を溶剤に溶かした
溶剤型接着剤等があげられる。また、水ガラス、エナメ
ル、うわぐすり等の無機化合物接着剤でもよい。The binder used in the present invention is not particularly limited. Specific examples include a synthetic resin emulsion adhesive, a rubber latex adhesive, a solvent-type adhesive obtained by dissolving various rubbers and resins in a solvent, and the like. Further, an inorganic compound adhesive such as water glass, enamel and glaze may be used.
バインダーの使用量は、吸着剤及び多孔性基材の種類
及び量によっても異なるが、通常、吸着剤とバインダー
との重量比が、1:5〜20:1となる範囲である。バインダ
ー量が多すぎると脱臭性能が低下し、少なすぎると吸着
剤の多孔性基材への接着固定が不十分となる。The amount of the binder used varies depending on the types and amounts of the adsorbent and the porous base material, but is usually in a range where the weight ratio between the adsorbent and the binder is 1: 5 to 20: 1. If the amount of the binder is too large, the deodorizing performance is reduced, and if the amount is too small, the adsorbent is insufficiently adhered and fixed to the porous substrate.
多孔性基材と吸着剤とを接着固定する方法は、従来公
知の方法でよい。例えば、あらかじめ多孔性基材にバイ
ンダーを含浸あるいは塗布した後、吸着剤をその表面に
散布して固着させる方法が用いられる。また、吸着剤を
分散させた合成樹脂エマルジョンなどを多孔性基材に含
浸又は塗布する等の方法によってもよい。The method of bonding and fixing the porous substrate and the adsorbent may be a conventionally known method. For example, a method of impregnating or applying a binder to a porous base material in advance, and then scattering and adsorbing an adsorbent on the surface is used. Alternatively, the porous substrate may be impregnated or coated with a synthetic resin emulsion or the like in which an adsorbent is dispersed.
本発明の方法においては、多孔性基材にバインダーで
吸着剤を接着固定した後、更に硫酸アルミニウム及び遷
移金属の硫酸塩を含有させる。In the method of the present invention, after the adsorbent is bonded and fixed to the porous substrate with a binder, aluminum sulfate and a sulfate of a transition metal are further contained.
本発明において用いる硫酸アルミニウムは無水物でも
水和物でもよい。Aluminum sulfate used in the present invention may be anhydrous or hydrated.
本発明において用いる遷移金属の硫酸塩は、短周期型
周期律表のI B、II B、III B、IV B、V B、VI B、VII B
及びVIII族の金属の硫酸塩であればよいが、中でも第一
遷移系列元素の硫酸塩、とりわけ、銅、亜鉛、鉄、コバ
ルト、ニッケルの硫酸塩が好ましい。これらの遷移金属
の硫酸塩は、一種類単独で使用してもよく、また、二種
類以上を併用してもよい。The sulfate of the transition metal used in the present invention is IB, IIB, IIIB, IVB, VB, VIB, VIIB of the periodic table of the short period type.
And VIII-group metal sulfates, among which sulfates of the first transition series elements, particularly sulfates of copper, zinc, iron, cobalt and nickel, are preferred. These transition metal sulfates may be used alone or in a combination of two or more.
硫酸アルミニウムと遷移金属硫酸塩の配合比は適宜選
択しうるが、通常は硫酸アルミニウムと遷移金属硫酸塩
の重量比が無水塩換算で100:1〜1:2、好ましくは10:1〜
1:1の範囲である。この比を極端に外れると吸着剤の脱
落が起きたり、硫酸アルミニウム及び遷移金属の硫酸塩
の多孔性基材への付着が弱くなったりする。The mixing ratio of aluminum sulfate and transition metal sulfate can be appropriately selected, but usually, the weight ratio of aluminum sulfate and transition metal sulfate is 100: 1 to 1: 2 in terms of anhydrous salt, preferably 10: 1 to
The range is 1: 1. If the ratio is extremely outside the above range, the adsorbent may fall off, or the adhesion of aluminum sulfate and sulfate of transition metal to the porous substrate may be weakened.
本発明の脱臭性複合材料の製造方法において、硫酸ア
ルミニウム及び遷移金属の硫酸塩は、その合計重量(無
水塩換算)と吸着剤との重量比率が1:100〜1:2、好まし
くは1:100〜1:5になるように使用する。In the method for producing a deodorizable composite material of the present invention, the aluminum sulfate and the sulfate of the transition metal have a total weight (in terms of anhydrous salt) and a weight ratio of the adsorbent of 1: 100 to 1: 2, preferably 1: 1: Use so that it becomes 100-1: 5.
本発明の脱臭性複合材料の製造方法においては、多孔
性基材にバインダーで吸着剤を接着固定した後、更に硫
酸アルミニウム及び遷移金属の硫酸塩を含有させる。本
発明の方法において、吸着剤が固定された多孔性基材に
又は多孔性基材に固定された吸着剤に硫酸塩を含有させ
る方法は、特に限定されないが、通常、硫酸アルミニウ
ム及び遷移金属の硫酸塩の溶液に含浸する、スプレーで
噴霧する、又は水溶液を塗布する等の方法が採用でき
る。これらの方法において、硫酸アルミニウムと遷移金
属の硫酸塩とは、必ずしも同時に含有させる必要はな
い。なお、必要に応じて、多孔性基材又は吸着剤に硫酸
塩を含有させた後、加熱して、含浸等に使用した溶媒を
除去することもできる。In the method for producing a deodorizable composite material of the present invention, an adsorbent is adhered and fixed to a porous substrate with a binder, and further contains aluminum sulfate and a sulfate of a transition metal. In the method of the present invention, the method of including a sulfate in the porous substrate to which the adsorbent is fixed or in the adsorbent fixed to the porous substrate is not particularly limited, but usually, aluminum sulfate and transition metal A method of impregnating with a sulfate solution, spraying with a spray, or applying an aqueous solution can be employed. In these methods, it is not always necessary to simultaneously contain aluminum sulfate and a sulfate of a transition metal. If necessary, after the sulfate is contained in the porous substrate or the adsorbent, the solvent used for the impregnation or the like can be removed by heating.
上記方法によれば、吸着剤の脱落が少ない脱臭性複合
材料を得ることができる。According to the above method, it is possible to obtain a deodorizable composite material in which the adsorbent is less likely to fall off.
本発明の脱臭性複合材料の製造方法においては、本発
明の効果を損なわない限りであれば既存の脱臭剤、消臭
剤、殺菌剤、防カビ剤を併用することができる。In the method for producing a deodorizable composite material of the present invention, existing deodorants, deodorants, germicides, and fungicides can be used in combination as long as the effects of the present invention are not impaired.
(発明の効果) 本発明の脱臭性複合材料の製造方法によれば、従来技
術に比較して、吸着剤の脱落が少なく、加えて脱臭性能
も更に優れた脱臭性複合材料を得ることができる。(Effect of the Invention) According to the method for producing a deodorizing composite material of the present invention, a deodorizing composite material can be obtained in which the adsorbent is less likely to fall off and the deodorizing performance is more excellent than in the prior art. .
本発明の方法で得られた吸着性複合材料は、単独であ
るいは他の多孔性基材や吸着材と組み合わせたり、エレ
クトレット不織布等と組み合わせて空気清浄機等の脱臭
フィルターとして用いることができるほか、各種脱臭用
及び吸着用の素材として幅広く利用が可能である。The adsorptive composite material obtained by the method of the present invention can be used alone or in combination with another porous substrate or adsorbent, or in combination with an electret nonwoven fabric or the like, and can be used as a deodorizing filter such as an air purifier, It can be widely used as a material for deodorization and adsorption.
(実施例) 以下に実施例を挙げて本発明を更に具体的に説明す
る。なお、実施例及び比較例中の部及び%は、特に断り
のないかぎり重量基準である。また、ラテックス重量は
固形分換算である。(Example) Hereinafter, the present invention will be described more specifically with reference to examples. Parts and% in Examples and Comparative Examples are based on weight unless otherwise specified. The weight of the latex is in terms of solid content.
実施例1 多孔性基材として三次元骨格を有するポリウレタンフ
ォーム(エバーライトスコットHR−08、サイズ厚さ10mm
×縦100mm×横100mm、重量2.8g、ブリヂストン社)に、
アクリレートラテックス(Nipol LX825、日本ゼオン社
製)2gを塗布した。これに吸着剤として、椰子殻活性炭
(ダイアソーブ−W、30−60メッシュ、三菱化成工業社
製)6gを均一に散布し付着させた後、120℃で30分乾燥
した。次いで、硫酸アルミニウム(13〜14水塩、キシダ
化学社製、1級)18部及び硫酸銅・5水塩2部を80部の
水に溶解して得た20%水溶液に含浸したのち、120℃で3
0分乾燥して、硫酸塩を1.0g(無水塩換算)含有した脱
臭性複合材料1を得た。Example 1 Polyurethane foam having a three-dimensional skeleton as a porous substrate (Everlight Scott HR-08, size thickness 10 mm)
× length 100mm × width 100mm, weight 2.8g, Bridgestone)
2 g of acrylate latex (Nipol LX825, manufactured by Zeon Corporation) was applied. As an adsorbent, 6 g of coconut shell activated carbon (Diasorb-W, 30-60 mesh, manufactured by Mitsubishi Kasei Kogyo Co., Ltd.) was uniformly dispersed and adhered, and then dried at 120 ° C. for 30 minutes. Next, 18 parts of aluminum sulfate (13-14 hydrate, manufactured by Kishida Chemical Co., Ltd., first grade) and 2 parts of copper sulfate pentahydrate are dissolved in 80 parts of water, and impregnated with a 20% aqueous solution. 3 in ℃
After drying for 0 minutes, a deodorizable composite material 1 containing 1.0 g of sulfate (in terms of anhydrous salt) was obtained.
実施例2〜7 硫酸アルミニウムの量、遷移金属の硫酸塩の種類又は
量を第1表に示すように変えるほかは、実施例1と同様
にして、脱臭性複合材料2〜7を得た。Examples 2 to 7 Deodorizing composite materials 2 to 7 were obtained in the same manner as in Example 1 except that the amount of aluminum sulfate and the type or amount of the sulfate of the transition metal were changed as shown in Table 1.
実施例8 ポリウレタンフォームに代えて不織布(繊維径15デニ
ールのナイロン不織布、厚さ10mm×縦100mm×横100mm、
重量2.0g)を用いるほかは実施例1と同様にして脱臭性
複合材料8を得た。Example 8 In place of polyurethane foam, a nonwoven fabric (a nylon nonwoven fabric having a fiber diameter of 15 denier, thickness 10 mm × length 100 mm × width 100 mm,
A deodorant composite material 8 was obtained in the same manner as in Example 1 except that the weight was 2.0 g).
実施例9 吸着剤としてシリカゲル(マイクロ・ビーズ・シリカ
ゲル、30−200メッシュ、富士デヴィソン化学(株)
製)を用いる以外は実施例1と同様にして脱臭性複合材
料9を得た。Example 9 Silica gel (microbead silica gel, 30-200 mesh, Fuji Devison Chemical Co., Ltd.) as an adsorbent
Deodorizing composite material 9 was obtained in the same manner as in Example 1 except for using
実施例10 吸着剤として椰子殻活性炭(ダイアソーブ−F、100
メッシュ以下、三菱化成工業(株)製)1gを用い、硫酸
塩担持量を0.2gとする他は実施例2と同様にして脱臭性
複合材料10を得た。Example 10 Coconut shell activated carbon (Diasorb-F, 100
A deodorizable composite material 10 was obtained in the same manner as in Example 2, except that 1 g of a mesh or less (manufactured by Mitsubishi Kasei Kogyo Co., Ltd.) was used and the amount of sulfate carried was 0.2 g.
実施例11 活性炭の量を0.5g、LX825の量を2gとし、硫酸塩担持
量を0.1gとする他は実施例10と同様にして脱臭性複合材
料11を得た。Example 11 A deodorizable composite material 11 was obtained in the same manner as in Example 10, except that the amount of activated carbon was 0.5 g, the amount of LX825 was 2 g, and the amount of sulfate carried was 0.1 g.
比較例1〜5 第1表に示す多孔性基材を使用し、硫酸アルミニウム
及び/又は遷移金属の硫酸塩を使用しないほかは、実施
例1と同様にして、脱臭性複合材料12〜16を得た。Comparative Examples 1 to 5 Deodorizing composite materials 12 to 16 were prepared in the same manner as in Example 1 except that the porous substrates shown in Table 1 were used and aluminum sulfate and / or a sulfate of a transition metal were not used. Obtained.
実施例12 上記各実施例で得た各脱臭性複合材料を裁断して作製
した試験片(厚さ10mm×縦10mm×横25mm、但し、実験番
号10及び11については、それぞれ、厚さ10mm×縦60mm×
横25mm、厚さ10mm×縦100mm×横50mmのものを用い
た。)を150mlのガラス容器に入れた後、内部を5%の
アンモニアガスを含む空気で置換し、直ちに密閉した。
2時間静置後に気相部分のアンモニア量をガスクロマト
グラフで測定してアンモニア脱臭性能を評価した。Example 12 A test piece prepared by cutting each deodorizing composite material obtained in each of the above Examples (thickness: 10 mm × length: 10 mm × width: 25 mm; for Experiment Nos. 10 and 11, respectively, the thickness was 10 mm × Length 60mm ×
Those having a width of 25 mm, a thickness of 10 mm, a length of 100 mm and a width of 50 mm were used. ) Was placed in a 150 ml glass container, the inside was replaced with air containing 5% ammonia gas, and the container was immediately sealed.
After standing for 2 hours, the amount of ammonia in the gas phase was measured by gas chromatography to evaluate the ammonia deodorizing performance.
また、同様にして5%の硫化水素を含む空気を用いて
硫化水素脱臭性能を評価した。この結果を第1表に示
す。In the same manner, hydrogen sulfide deodorizing performance was evaluated using air containing 5% hydrogen sulfide. Table 1 shows the results.
また、各脱臭性複合材料から作製した試験片(厚さ10
mm×縦50mm×横100mm)の両端を持って10回揉み擦った
ときの吸着剤の脱落量を調べた。その結果を併せて第1
表に示す。In addition, test specimens (thickness 10
(mm x 50 mm x 100 mm) were rubbed and rubbed 10 times, and the amount of adsorbent dropped off was examined. Based on the results,
It is shown in the table.
第1表の結果から、本発明の方法で得られた脱臭性複
合材料は、脱臭性能に優れ、かつ吸着剤の脱落も少ない
のに対して、硫酸アルミニウム及び/又は遷移金属の硫
酸塩を用いない場合は、脱臭性能も劣り、かつ吸着剤の
脱落が多いことが分かる。 From the results in Table 1, it can be seen that the deodorizing composite material obtained by the method of the present invention has excellent deodorizing performance and has a small amount of adsorbent, while using aluminum sulfate and / or a sulfate of a transition metal. If no, the deodorizing performance is inferior and the adsorbent often drops off.
Claims (1)
定し、次いで硫酸アルミニウム及び遷移金属の硫酸塩を
含有させることを特徴とする脱臭性複合材料の製造方
法。1. A method for producing a deodorizable composite material, comprising adhering and fixing an adsorbent to a porous substrate with a binder, and then adding aluminum sulfate and a sulfate of a transition metal.
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
JP2222202A JP2583151B2 (en) | 1990-08-23 | 1990-08-23 | Method for producing deodorant composite material |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
JP2222202A JP2583151B2 (en) | 1990-08-23 | 1990-08-23 | Method for producing deodorant composite material |
Publications (2)
Publication Number | Publication Date |
---|---|
JPH04104835A JPH04104835A (en) | 1992-04-07 |
JP2583151B2 true JP2583151B2 (en) | 1997-02-19 |
Family
ID=16778738
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
JP2222202A Expired - Lifetime JP2583151B2 (en) | 1990-08-23 | 1990-08-23 | Method for producing deodorant composite material |
Country Status (1)
Country | Link |
---|---|
JP (1) | JP2583151B2 (en) |
Families Citing this family (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
TW422724B (en) * | 1997-07-03 | 2001-02-21 | Takasago Thermal Engineering | An air filter, the manufacturing method, and a high efficiency air cleaning apparatus |
JP3977514B2 (en) * | 1998-05-26 | 2007-09-19 | 高砂熱学工業株式会社 | Air purification filter, method of manufacturing the same, and advanced cleaning device |
DE10002400B4 (en) * | 2000-01-20 | 2008-06-12 | Raimund Homberg | Method and device for deodorizing room air, in particular for refrigerators |
KR20040000691A (en) * | 2002-06-25 | 2004-01-07 | 크린에어테크놀로지 주식회사 | Method for preparing porous deodorization filter adhering adhesive |
Family Cites Families (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JPS5274589A (en) * | 1975-12-18 | 1977-06-22 | Mitsubishi Heavy Ind Ltd | Porous substance for deodorization |
JPS5648242A (en) * | 1979-09-27 | 1981-05-01 | Oribesuto Kk | Production of adsorbable sheet |
-
1990
- 1990-08-23 JP JP2222202A patent/JP2583151B2/en not_active Expired - Lifetime
Also Published As
Publication number | Publication date |
---|---|
JPH04104835A (en) | 1992-04-07 |
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