JP3198185B2 - Mold production method - Google Patents
Mold production methodInfo
- Publication number
- JP3198185B2 JP3198185B2 JP02072193A JP2072193A JP3198185B2 JP 3198185 B2 JP3198185 B2 JP 3198185B2 JP 02072193 A JP02072193 A JP 02072193A JP 2072193 A JP2072193 A JP 2072193A JP 3198185 B2 JP3198185 B2 JP 3198185B2
- Authority
- JP
- Japan
- Prior art keywords
- mold
- resin
- alkyd resin
- parts
- refractory aggregate
- 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
Landscapes
- Mold Materials And Core Materials (AREA)
Description
【０００１】[0001]
【産業上の利用分野】本発明は、製造直後の引っ張り強
度や離型性等の諸性能に優れた鋳造用の鋳型を製造する
方法に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method for producing a casting mold excellent in various properties such as tensile strength and releasability immediately after production.
【０００２】[0002]
【従来の技術】従来、鋳造用の鋳型の工業的製造方法と
しては、その製造に際し加熱を必要としないため、エネ
ルギー消費の点で有利なアシュランド法（例えば、コー
ルドボックス法、ノーべーク法）が知られている。例と
して、アシュランドコールドボックス法による鋳型の製
造方法について説明する。まず、フェノール樹脂溶液、
ポリイソシアネート化合物溶液及び粒状耐火性骨材をミ
キサーで混合して粘結剤で被覆された粒状耐火性骨材を
調製し、これを鋳型製造用の型枠内に吹き込んで成形す
る。次に、この型枠内に第三級アミン等の硬化触媒を透
過させることにより常温で硬化させ脱型して、鋳造用の
鋳型を製造する。2. Description of the Related Art Conventionally, as an industrial production method of a casting mold, an Ashland method (for example, a cold box method, a no-bake method, or the like) which is advantageous in terms of energy consumption because heating is not required for its production. Law) is known. As an example, a method of manufacturing a mold by the Ashland cold box method will be described. First, a phenolic resin solution,
The polyisocyanate compound solution and the granular refractory aggregate are mixed by a mixer to prepare a granular refractory aggregate coated with a binder, and the mixture is blown into a mold for mold production to be molded. Next, a curing catalyst such as a tertiary amine is allowed to permeate into the mold to cure at room temperature and to be released from the mold to produce a casting mold.
【０００３】[0003]
【発明が解決しようとする課題】しかしながら、前記従
来の方法により製造した鋳造用の鋳型には、その製造直
後の引っ張り強度が十分でないため、例えば複雑な形状
を有する中子あるいは細い腕や脚を持つ鋳型は、脱型後
直ちに移設のため持ち運ぶ際に、あるいは鋳造のためそ
の設置の際に、変形、破損しやすいという問題点があ
る。この鋳型製造直後の変形、破損を防止するために
は、鋳型をその製造後数時間から一昼夜程度放置すれば
よいが、このような従来の方法では鋳物の製造効率が著
しく低い。本発明は、鋳型製造直後の引っ張り強度を改
善することにより、高い初期引っ張り強度を要する例え
ば複雑な形状の鋳型、ひいては鋳物を効率的に製造する
ことのできる方法を提供することを目的とする。However, since the casting mold manufactured by the above-mentioned conventional method has insufficient tensile strength immediately after its manufacture, for example, a core having a complicated shape or a thin arm or leg is required. The mold has a problem that it is easily deformed and damaged when it is carried for relocation immediately after demolding, or when it is installed for casting. In order to prevent the deformation and breakage immediately after the production of the mold, the mold may be left for several hours to one day and night after the production, but the production efficiency of the casting is extremely low in such a conventional method. An object of the present invention is to provide a method capable of efficiently producing a mold having a high initial tensile strength, for example, a mold having a complicated shape and thus a casting by improving the tensile strength immediately after the production of the mold.
【０００４】[0004]
【課題を解決するための手段】前記目的を達成するため
に、本発明の鋳型の製造方法は、フェノール樹脂、アル
キッド樹脂、ポリイソシアネート化合物、シラン化合
物、可使時間延長剤及び溶剤を含む粘結剤により被覆さ
れた粒状耐火性骨材を型枠内に導入して成形し、次いで
前記型枠内に硬化触媒を導入して硬化させることを特徴
とする。In order to achieve the above-mentioned object, a method for producing a mold according to the present invention comprises a phenol resin, an alkyd resin, a polyisocyanate compound, a silane compound, a binder containing a pot life extender and a solvent. The method is characterized in that the granular refractory aggregate coated with the agent is introduced into a mold and molded, and then a curing catalyst is introduced into the mold and cured.
【０００５】本発明において使用されるフェノール樹脂
は、フェノール類とホルムアルデヒドとの付加・縮合で
得られ、アシュランド法で通常使用される有機溶剤溶解
性のベンジルエーテル樹脂、レゾール樹脂あるいはノボ
ラック樹脂である。The phenolic resin used in the present invention is a benzyl ether resin, a resol resin or a novolak resin which is obtained by addition and condensation of phenols and formaldehyde and is generally used in the Ashland method and which is soluble in an organic solvent. .
【０００６】本発明において使用されるアルキッド樹脂
は、多価アルコールと多塩基酸との縮合によって得られ
る不飽和ポリエステル樹脂であり、この縮合の際に不飽
和脂肪酸、石油樹脂、フェノール、ウレタン、エポキ
シ、ビニルモノマー等で変性した変性アルキッド樹脂を
含む。この多価アルコールとしては、エチレングリコー
ル、プロピレングリコール、ジエチレングリコール、ト
リエチレングリコール、グリセリン、ペンタエリスリッ
ト等を挙げることができる。多塩基酸としては、無水フ
タル酸、無水マレイン酸、イソフタル酸、テトラクロロ
無水フタル酸、フマル酸、コハク酸、アジピン酸等を挙
げることができる。変性アルキッド樹脂としては、具体
的には、トール油脂肪酸変性アルキッド樹脂（ガードナ
ー粘度Ｔ〜Ｖ、酸価７＞）、アマニ油変性アルキッド樹
脂（ガードナー粘度Ｚ1 〜Ｚ2 、酸価１０＞）、アマニ
油及びウレタン化油変性アルキッド樹脂（不揮発分５０
％、ガードナー粘度Ｚ1 〜Ｚ3 、酸価０．５＞）、脱水
ヒマシ油脂肪酸及びエポキシエステル変性アルキッド樹
脂（不揮発分５０％、ガードナー粘度Ｕ〜Ｗ、酸価０．
５＞）、アマニ油及びアクリル化変性アルキッド樹脂
（不揮発分５３％、ガードナー粘度Ｕ〜Ｗ、酸価７
＞）、アマニ油及びフェノール化変性アルキッド樹脂
（不揮発分５５％、ガードナー粘度Ｗ〜Ｚ、酸価８＞）
等を挙げることができる。The alkyd resin used in the present invention is an unsaturated polyester resin obtained by condensation of a polyhydric alcohol and a polybasic acid. In this condensation, unsaturated fatty acid, petroleum resin, phenol, urethane, epoxy And modified alkyd resins modified with vinyl monomers and the like. Examples of the polyhydric alcohol include ethylene glycol, propylene glycol, diethylene glycol, triethylene glycol, glycerin, and pentaerythritol. Examples of the polybasic acid include phthalic anhydride, maleic anhydride, isophthalic acid, tetrachlorophthalic anhydride, fumaric acid, succinic acid, adipic acid and the like. Specific examples of the modified alkyd resin include tall oil fatty acid-modified alkyd resin (Gardner viscosity T to V, acid value 7>), linseed oil-modified alkyd resin (Gardner viscosity Z 1 to Z 2 , acid value 10>), Linseed oil and urethanized oil-modified alkyd resin (nonvolatile content 50
%, Gardner viscosity Z 1 to Z 3 , acid value 0.5>), dehydrated castor oil fatty acid and epoxy ester-modified alkyd resin (nonvolatile content 50%, Gardner viscosity U to W, acid value 0.
5>), linseed oil and acrylated modified alkyd resin (53% non-volatile content, Gardner viscosity U to W, acid value 7)
>), Linseed oil and phenolated modified alkyd resin (55% non-volatile content, Gardner viscosity W to Z, acid value 8>)
And the like.
【０００７】ポリイソシアネート化合物としては、公知
の芳香族、脂肪族あるいは脂環式のポリイソシアネート
を使用することができ、具体的には例えば、ジフェニル
メタンジイソシアネート、ポリメチレンポリフェニレン
ポリイソシアネート（以下ポリメックＭＤＩという）、
ヘキサメチレンジイソシアネート、４，４′−ジシクロ
ヘキシルメタンジイソシアネートを挙げることができ
る。As the polyisocyanate compound, known aromatic, aliphatic or alicyclic polyisocyanates can be used. Specifically, for example, diphenylmethane diisocyanate, polymethylene polyphenylene polyisocyanate (hereinafter referred to as Polymec MDI) ,
Hexamethylene diisocyanate and 4,4'-dicyclohexylmethane diisocyanate can be mentioned.
【０００８】粘結剤用の溶剤としては、アシュランド法
における粘結剤被覆粒状耐火性骨材の調製において使用
される溶剤は、いずれも本発明において使用することが
できる。具体的には、脂肪族炭化水素系、脂環式炭化水
素系、芳香族炭化水素系、ハロゲン化炭化水素系、ケト
ン系、エステル系、エーテル系、アルコール系等の有機
溶剤を単独でまたは混合して使用することができる。さ
らに、本発明の粘結剤溶液は、樹脂成分と骨材との接着
性の向上を図るため３−グリシドキシプロピルトリメト
キシシラン等のシラン化合物、可使時間延長剤としてイ
ソフタル酸クロリドを代表例とする酸クロリドを含むほ
か、所望により、劣化防止剤、乾燥防止剤、離型剤等を
含むことができる。As the solvent for the binder, any solvent used in the preparation of the binder-coated granular refractory aggregate in the Ashland method can be used in the present invention. Specifically, organic solvents such as aliphatic hydrocarbons, alicyclic hydrocarbons, aromatic hydrocarbons, halogenated hydrocarbons, ketones, esters, ethers, and alcohols are used alone or in combination. Can be used. Further, the binder solution of the present invention is represented by silane compounds such as 3-glycidoxypropyltrimethoxysilane and isophthalic acid chloride as a pot life extender in order to improve the adhesiveness between the resin component and the aggregate. In addition to the acid chloride as an example, if desired, a deterioration inhibitor, an anti-drying agent, a release agent and the like can be contained.
【０００９】本発明において使用される粒状耐火性骨材
は、具体的には例えば、微粉状の砂、粘土質の砂、再生
砂等を含むあらゆる種類の砂であるが、通常の鋳物砂が
好ましく、５０〜６００μ程度の砂が特に好ましい。フ
ェノール樹脂、ポリイソシアネート化合物あるいは溶剤
各々の粒状耐火性骨材に対する配合割合は、鋳型の硬化
性の改善及び強度確保の点から、それぞれ粒状耐火性骨
材に対し全て０．０１〜１０重量％の範囲が好ましく、
特に０．１〜５．０重量％の範囲が好ましい。アルキッ
ド樹脂は、フェノール樹脂あるいはポリイソシアネート
化合物（固形分）１００重量部に対して、０．５〜２０
重量部の範囲の量を使用するのが好ましく、１〜１０重
量部の範囲の量を使用するのが特に好ましい。The granular refractory aggregate used in the present invention is, for example, any kind of sand including fine powder sand, clay sand, and recycled sand. Sand of about 50 to 600 μm is particularly preferred. The mixing ratio of the phenolic resin, the polyisocyanate compound, or the solvent to the granular refractory aggregate is 0.01 to 10% by weight for the granular refractory aggregate, respectively, from the viewpoint of improving the curability of the mold and securing the strength. Range is preferred,
Particularly, the range of 0.1 to 5.0% by weight is preferable. The alkyd resin is used in an amount of 0.5 to 20 with respect to 100 parts by weight of the phenol resin or the polyisocyanate compound (solid content).
It is preferred to use amounts in the range of parts by weight, particularly preferred to use amounts in the range of 1 to 10 parts by weight.
【００１０】粘結剤被覆粒状耐火性骨材の調製は、例え
ば、フェノール樹脂、アルキッド樹脂、ポリイソシアネ
ート化合物、シラン化合物、可使時間延長剤及び溶剤か
ら成る粘結剤溶液と粒状耐火性骨材とを、好ましくは−
１０〜５０℃の範囲の温度で、ミキサーにより各成分が
均一に混合するように十分に混練することによって行な
うことができる。粘結剤溶液の調製には、あらかじめフ
ェノール樹脂溶液とイソシアネート化合物溶液とを別々
に調製し、いずれか一方又は双方にアルキッド樹脂、シ
ラン化合物及び可使時間延長剤を添加しておくか、ある
いはこれらの溶液とは別にアルキッド樹脂、シラン化合
物及び可使時間延長剤の溶液を調製しておき、粒状耐火
性骨材との混練時に、これらの溶液を粒状耐火性骨材に
添加してもよい。調製した粘結剤被覆粒状耐火性骨材
を、例えば、サンドマガジン内に貯留し、エアーによる
吹き込みによってその所望量を鋳型製造用型枠内に導入
し、次いで、塩基、アミン、金属イオン等のアシュラン
ド法において通常使用される硬化触媒を前記型枠内に導
入し、脱型することによって、鋳型を製造する。The preparation of the binder-coated granular refractory aggregate includes, for example, a binder solution comprising a phenol resin, an alkyd resin, a polyisocyanate compound, a silane compound, a pot life extending agent and a solvent, and a particulate refractory aggregate. And preferably-
The mixing can be carried out by sufficiently kneading the components at a temperature in the range of 10 to 50 ° C so that the components are uniformly mixed. For the preparation of the binder solution, a phenol resin solution and an isocyanate compound solution are separately prepared in advance, and an alkyd resin, a silane compound and a pot life extender are added to one or both of them, or A solution of an alkyd resin, a silane compound, and a pot life extender may be prepared separately from the above solution, and these solutions may be added to the granular refractory aggregate at the time of kneading with the granular refractory aggregate. The prepared binder-coated granular refractory aggregate, for example, is stored in a sand magazine, the desired amount is introduced into the mold for mold production by blowing with air, and then the base, amine, metal ions, etc. A mold is manufactured by introducing a curing catalyst generally used in the Ashland method into the mold and demolding.
【００１１】[0011]
【実施例】以下、実施例及び比較例により本発明をさら
に詳細に説明する。以下、「部」は全て「重量部」を意
味する。実施例１〜３ まず、保土谷化学工業株式会社製ベンジルエーテル基含
有フェノール樹脂５０部、二塩基酸メチルエステル混合
物（コハク酸ジメチル：グルタル酸ジメチル：アジピン
酸ジメチル＝２５部：５５部：２０部、デュポン社製Ｄ
ＢＥ）２０部、石油系溶剤（丸善石油株式会社製ＳＷ−
１８００）３０部及び３−グリシドキシプロピルトリメ
トキシシラン０．３部から成る溶液を調製した。別に、
ポリメリックＭＤＩ７５部、石油系溶剤（出光興産株式
会社製ＩＰ−１５０）２５部及びイソフタル酸クロリド
０．５部から成る溶液を調製した。この溶液中に、前記
ポリメリックＭＤＩ５０部に対して、表１に示す所定量
のアマニ油変性アルキッド樹脂ハリフタールＳＬ−８８
９（ハリマ化成株式会社製）を添加して溶解させた。フ
リーマントル珪砂１００部に対して、前記フェノール樹
脂溶液と変性アルキッド樹脂を含む前記ポリイソシアネ
ート溶液とをそれぞれ０．９部の比率で添加し、品川式
ミキサーで９０秒間混練した。この粘結剤被覆砂をドッ
グボーン形砂型用金型をとりつけた浪速製作所製Ｖ−Ｔ
ＯＰ３３０Ｃコールドボックス造型機のサンドマガジン
内に移し、サンドマガジン内に３．０ｋｇｆ／ｃｍ2 の
ゲージ圧でブローしてドッグボーン形砂型用金型に吹き
込んだ。次に、トリエチルアミンガスジェネレーターに
より２．５ｋｇｆ／ｃｍ2 のゲージ圧で１秒間ガッシン
グし、前記金型内にトリエチルアミンを透過させてキュ
アリングした後、３．０ｋｇｆ／ｃｍ2 のゲージ圧で３
秒間エアーパージし脱型してドッグボーン形砂型を製造
し、この砂型の密度と引っ張り強度を測定した。製造し
た鋳型（砂型）の性能を表１に示す。The present invention will be described in more detail with reference to the following Examples and Comparative Examples. Hereinafter, all “parts” mean “parts by weight”. Examples 1 to 3 First, 50 parts of a benzyl ether group-containing phenol resin manufactured by Hodogaya Chemical Co., Ltd., and a mixture of dibasic acid methyl esters (dimethyl succinate: dimethyl glutarate: dimethyl adipate = 25 parts: 55 parts: 20 parts) , Made by Dupont
(BE) 20 parts, petroleum-based solvent (SW- manufactured by Maruzen Oil Co., Ltd.)
1800) 30 parts and 0.3 parts of 3-glycidoxypropyltrimethoxysilane. Separately,
A solution comprising 75 parts of polymeric MDI, 25 parts of a petroleum-based solvent (IP-150 manufactured by Idemitsu Kosan Co., Ltd.) and 0.5 parts of isophthalic acid chloride was prepared. In this solution, a predetermined amount of linseed oil-modified alkyd resin Khalyphtal SL-88 shown in Table 1 was added to 50 parts of the polymeric MDI.
9 (manufactured by Harima Chemicals, Inc.) was added and dissolved. To 100 parts of Fremantle silica sand, the phenol resin solution and the polyisocyanate solution containing the modified alkyd resin were added at a ratio of 0.9 parts, respectively, and kneaded with a Shinagawa mixer for 90 seconds. VT manufactured by Naniwa Seisakusho with this binder-coated sand attached to a dogbone type sand mold.
It was transferred into a sand magazine of an OP330C cold box molding machine, blown into the sand magazine at a gauge pressure of 3.0 kgf / cm 2 , and blown into a dogbone type sand mold. Then, the triethylamine gas generator and gassing for 1 second at a gauge pressure of 2.5 kgf / cm 2, and curing by transmitting triethylamine in the mold, 3 a gauge pressure of 3.0 kgf / cm 2
A dog bone type sand mold was manufactured by air purging for 2 seconds and the mold was removed, and the density and tensile strength of the sand mold were measured. Table 1 shows the performance of the produced mold (sand mold).
【表１】 表１より、鋳型の密度等の性能を低下させることなく、
その初期（特に製造３０秒後）引っ張り強度を著しく改
善することができた。また、離型性も著しく改善され
た。[Table 1] From Table 1, without reducing the performance such as the density of the mold,
Its initial (especially after 30 seconds of production) tensile strength was significantly improved. In addition, the releasability was significantly improved.
【００１２】実施例４及び５ 実施例１において、ポリメリックＭＤＩを含む溶液中に
おいてアマニ油変性アルキッド樹脂のみを含まない溶液
を使用し、フェノール樹脂を含む溶液中に、フェノール
樹脂５０部に対して表２に示す所定量のアマニ油変性ア
ルキッド樹脂リノキュアパートＡ（保土谷アシュランド
株式会社製）を添加した溶液を使用した以外は、実施例
１と同様にして鋳型を製造した。製造した鋳型の性能を
表２に示す。 Examples 4 and 5 In Example 1, a solution containing only linseed oil-modified alkyd resin was used in a solution containing polymeric MDI, and a solution containing 50 parts of phenol resin was used in a solution containing phenol resin. A mold was produced in the same manner as in Example 1 except that a solution to which a predetermined amount of linseed oil-modified alkyd resin Linocupert A (Hodogaya Ashland Co., Ltd.) shown in No. 2 was added was used. Table 2 shows the performance of the manufactured molds.
【表２】 表２より、鋳型の密度等の性能を低下させることなく、
その初期（製造３０秒後）引っ張り強度を著しく改善す
ることができた。また、離型性も著しく改善された。比較例１ 実施例１において、アマニ油変性アルキッド樹脂を含ま
ないポリメリックＭＤＩ溶液を使用した以外は、実施例
１と同様にして鋳型を製造した。製造した鋳型の性能を
表１、表２に示す。[Table 2] From Table 2, without reducing the performance such as the density of the mold,
Its initial (30 seconds after production) tensile strength could be significantly improved. In addition, the releasability was significantly improved. Comparative Example 1 A mold was produced in the same manner as in Example 1 except that a polymeric MDI solution containing no linseed oil-modified alkyd resin was used. Tables 1 and 2 show the performance of the produced molds.
【００１３】[0013]
【発明の効果】以上説明した通り、本発明により、製造
直後（３０秒後）の鋳型の引っ張り強度を顕著に改善す
ることができると共に、鋳型製造時の離型性も併せて改
善することができる。その結果、高い初期引っ張り強度
を要する（中子を含む）鋳型、ひいては例えば複雑な形
状の鋳物を効率的に製造することが可能となった。さら
に、高品質の鋳物を製造することのできる、表面のなめ
らかな鋳型を提供することができる。As described above, according to the present invention, the tensile strength of the mold immediately after the production (after 30 seconds) can be remarkably improved, and the releasability at the time of the production of the mold can be also improved. it can. As a result, it has become possible to efficiently produce a mold (including a core) requiring a high initial tensile strength, and thus, for example, a casting having a complicated shape. Further, it is possible to provide a mold having a smooth surface capable of producing a high quality casting.
───────────────────────────────────────────────────── フロントページの続き (72)発明者 本間 司 神奈川県横浜市鶴見区大黒町７番43号 保土谷アシュランド株式会社 技術研究 所内 (56)参考文献 特開 昭60−87948（ＪＰ，Ａ) (58)調査した分野(Int.Cl.7，ＤＢ名) B22C 1/00 - 1/26 ──────────────────────────────────────────────────続 き Continued on the front page (72) Inventor Tsukasa Honma 7-43, Oguro-cho, Tsurumi-ku, Yokohama-shi, Kanagawa Prefecture Hodogaya Ashland Co., Ltd. Technical Research Institute (56) References JP-A-60-87948 (JP, A (58) Field surveyed (Int. Cl. 7 , DB name) B22C 1/00-1/26
Claims (2)
イソシアネート化合物、シラン化合物、可使時間延長剤
及び溶剤を含む粘結剤により被覆された粒状耐火性骨材
を型枠内に導入して成形し、次いで前記型枠内に硬化触
媒を導入して硬化させることを特徴とする鋳型の製造方
法。1. A particulate refractory aggregate coated with a binder containing a phenolic resin, an alkyd resin, a polyisocyanate compound, a silane compound, a pot life extending agent and a solvent is introduced into a mold, and molded. Next, a curing catalyst is introduced into the mold to cure the mold.
ポリイソシアネート化合物、シラン化合物、可使時間延
長剤及び溶剤を含む粘結剤により被覆された粒状耐火性
骨材を型枠内に導入して成形し、次いで前記型枠内に硬
化触媒を導入して硬化させることを特徴とする鋳型の製
造方法。2. A phenol resin, a modified alkyd resin,
A polyisocyanate compound, a silane compound, a granulated refractory aggregate coated with a binder containing a pot life extender and a solvent are introduced into a mold and molded, and then a curing catalyst is introduced into the mold. And producing a mold.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP02072193A JP3198185B2 (en) | 1993-01-14 | 1993-01-14 | Mold production method |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP02072193A JP3198185B2 (en) | 1993-01-14 | 1993-01-14 | Mold production method |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH06210390A JPH06210390A (en) | 1994-08-02 |
| JP3198185B2 true JP3198185B2 (en) | 2001-08-13 |
Family
ID=12035039
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP02072193A Expired - Lifetime JP3198185B2 (en) | 1993-01-14 | 1993-01-14 | Mold production method |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3198185B2 (en) |
Families Citing this family (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6232368B1 (en) * | 1999-10-12 | 2001-05-15 | Borden Chemical, Inc. | Ester cured binders |
-
1993
- 1993-01-14 JP JP02072193A patent/JP3198185B2/en not_active Expired - Lifetime
Also Published As
| Publication number | Publication date |
|---|---|
| JPH06210390A (en) | 1994-08-02 |
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