JPH04100B2 - - Google Patents
Info
- Publication number
- JPH04100B2 JPH04100B2 JP1272037A JP27203789A JPH04100B2 JP H04100 B2 JPH04100 B2 JP H04100B2 JP 1272037 A JP1272037 A JP 1272037A JP 27203789 A JP27203789 A JP 27203789A JP H04100 B2 JPH04100 B2 JP H04100B2
- Authority
- JP
- Japan
- Prior art keywords
- weight
- parts
- rubber
- rubber composition
- curing agent
- 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
- 229920005989 resin Polymers 0.000 claims description 20
- 239000011347 resin Substances 0.000 claims description 20
- 239000000203 mixture Substances 0.000 claims description 14
- 239000003795 chemical substances by application Substances 0.000 claims description 11
- 229920001187 thermosetting polymer Polymers 0.000 claims description 10
- 239000004760 aramid Substances 0.000 claims description 9
- 229920003235 aromatic polyamide Polymers 0.000 claims description 9
- 239000011324 bead Substances 0.000 claims description 9
- 229920001875 Ebonite Polymers 0.000 claims description 8
- VKYKSIONXSXAKP-UHFFFAOYSA-N hexamethylenetetramine Chemical group C1N(C2)CN3CN1CN2C3 VKYKSIONXSXAKP-UHFFFAOYSA-N 0.000 claims description 4
- 229920003244 diene elastomer Polymers 0.000 claims description 3
- 229920001568 phenolic resin Polymers 0.000 claims description 3
- 239000005011 phenolic resin Substances 0.000 claims description 3
- KXGFMDJXCMQABM-UHFFFAOYSA-N 2-methoxy-6-methylphenol Chemical compound [CH]OC1=CC=CC([CH])=C1O KXGFMDJXCMQABM-UHFFFAOYSA-N 0.000 claims description 2
- QTWJRLJHJPIABL-UHFFFAOYSA-N 2-methylphenol;3-methylphenol;4-methylphenol Chemical compound CC1=CC=C(O)C=C1.CC1=CC=CC(O)=C1.CC1=CC=CC=C1O QTWJRLJHJPIABL-UHFFFAOYSA-N 0.000 claims description 2
- 229930003836 cresol Natural products 0.000 claims description 2
- 235000010299 hexamethylene tetramine Nutrition 0.000 claims description 2
- 239000004312 hexamethylene tetramine Substances 0.000 claims description 2
- 125000000160 oxazolidinyl group Chemical group 0.000 claims 1
- 229920001971 elastomer Polymers 0.000 description 14
- 239000005060 rubber Substances 0.000 description 14
- 238000004898 kneading Methods 0.000 description 4
- WYNCHZVNFNFDNH-UHFFFAOYSA-N Oxazolidine Chemical compound C1COCN1 WYNCHZVNFNFDNH-UHFFFAOYSA-N 0.000 description 3
- 239000000835 fiber Substances 0.000 description 3
- 238000004073 vulcanization Methods 0.000 description 3
- 239000004636 vulcanized rubber Substances 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 238000001125 extrusion Methods 0.000 description 2
- 125000001570 methylene group Chemical group [H]C([H])([*:1])[*:2] 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 230000003014 reinforcing effect Effects 0.000 description 2
- 229910052717 sulfur Inorganic materials 0.000 description 2
- 239000011593 sulfur Substances 0.000 description 2
- OYHQOLUKZRVURQ-NTGFUMLPSA-N (9Z,12Z)-9,10,12,13-tetratritiooctadeca-9,12-dienoic acid Chemical compound C(CCCCCCC\C(=C(/C\C(=C(/CCCCC)\[3H])\[3H])\[3H])\[3H])(=O)O OYHQOLUKZRVURQ-NTGFUMLPSA-N 0.000 description 1
- WRIDQFICGBMAFQ-UHFFFAOYSA-N (E)-8-Octadecenoic acid Natural products CCCCCCCCCC=CCCCCCCC(O)=O WRIDQFICGBMAFQ-UHFFFAOYSA-N 0.000 description 1
- LQJBNNIYVWPHFW-UHFFFAOYSA-N 20:1omega9c fatty acid Natural products CCCCCCCCCCC=CCCCCCCCC(O)=O LQJBNNIYVWPHFW-UHFFFAOYSA-N 0.000 description 1
- QSBYPNXLFMSGKH-UHFFFAOYSA-N 9-Heptadecensaeure Natural products CCCCCCCC=CCCCCCCCC(O)=O QSBYPNXLFMSGKH-UHFFFAOYSA-N 0.000 description 1
- 244000226021 Anacardium occidentale Species 0.000 description 1
- 244000043261 Hevea brasiliensis Species 0.000 description 1
- CTQNGGLPUBDAKN-UHFFFAOYSA-N O-Xylene Chemical compound CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 description 1
- ZQPPMHVWECSIRJ-UHFFFAOYSA-N Oleic acid Natural products CCCCCCCCC=CCCCCCCCC(O)=O ZQPPMHVWECSIRJ-UHFFFAOYSA-N 0.000 description 1
- 239000005642 Oleic acid Substances 0.000 description 1
- MBHRHUJRKGNOKX-UHFFFAOYSA-N [(4,6-diamino-1,3,5-triazin-2-yl)amino]methanol Chemical class NC1=NC(N)=NC(NCO)=N1 MBHRHUJRKGNOKX-UHFFFAOYSA-N 0.000 description 1
- 150000004996 alkyl benzenes Chemical group 0.000 description 1
- DTOSIQBPPRVQHS-PDBXOOCHSA-N alpha-linolenic acid Chemical compound CC\C=C/C\C=C/C\C=C/CCCCCCCC(O)=O DTOSIQBPPRVQHS-PDBXOOCHSA-N 0.000 description 1
- 235000020661 alpha-linolenic acid Nutrition 0.000 description 1
- 230000003712 anti-aging effect Effects 0.000 description 1
- 235000020226 cashew nut Nutrition 0.000 description 1
- 229920003193 cis-1,4-polybutadiene polymer Polymers 0.000 description 1
- 229920003211 cis-1,4-polyisoprene Polymers 0.000 description 1
- 238000013329 compounding Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 238000004132 cross linking Methods 0.000 description 1
- 230000002542 deteriorative effect Effects 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 239000000945 filler Substances 0.000 description 1
- 230000001771 impaired effect Effects 0.000 description 1
- QXJSBBXBKPUZAA-UHFFFAOYSA-N isooleic acid Natural products CCCCCCCC=CCCCCCCCCC(O)=O QXJSBBXBKPUZAA-UHFFFAOYSA-N 0.000 description 1
- 229960004488 linolenic acid Drugs 0.000 description 1
- KQQKGWQCNNTQJW-UHFFFAOYSA-N linolenic acid Natural products CC=CCCC=CCC=CCCCCCCCC(O)=O KQQKGWQCNNTQJW-UHFFFAOYSA-N 0.000 description 1
- 229920003052 natural elastomer Polymers 0.000 description 1
- 229920001194 natural rubber Polymers 0.000 description 1
- 239000003921 oil Substances 0.000 description 1
- ZQPPMHVWECSIRJ-KTKRTIGZSA-N oleic acid Chemical compound CCCCCCCC\C=C/CCCCCCCC(O)=O ZQPPMHVWECSIRJ-KTKRTIGZSA-N 0.000 description 1
- 235000021313 oleic acid Nutrition 0.000 description 1
- 150000002989 phenols Chemical class 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 239000004014 plasticizer Substances 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 230000002787 reinforcement Effects 0.000 description 1
- 238000010058 rubber compounding Methods 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- 238000005987 sulfurization reaction Methods 0.000 description 1
- 230000002194 synthesizing effect Effects 0.000 description 1
- 239000002966 varnish Substances 0.000 description 1
- 239000008096 xylene Substances 0.000 description 1
Description
本発明は硬質ゴム組成物、特にビードエイペツ
クスあるいはクリンチエイペツクスに好適な硬質
ゴム組成物に関するもので、更に詳しくは加硫可
能なジエン系ゴムに芳香族ポリアミドパルプと熱
硬化性樹脂及び硬化剤を配合してなる硬質ゴム組
成物に関する。
一般にラジアルタイヤはカーカスプライのコー
ドをタイヤ赤道面に対してほぼ直角に相互に平行
になるように配列するとともにその両端をビード
ワイヤのまわりに折り返し、このプライの折り返
し端とカーカスに囲まれる内側にサイドウオール
方向に延びるビードエイペツクスを配置するとと
もにプライの折り返しの外惻でリムフランジに隣
接する領域にクリンチエイペツクスが配置され
る。このようなラジアル構造のタイヤではプライ
の折り返し端部での剛性の段差が生じ、この部分
での損傷が起きやすく、またラジアル構造である
ことから本質的に横剛性が劣るという欠点があ
り、そのため前記ビードエイペツクスあるいはク
リンチエイペツクスに特に硬度(あるいは動的弾
性率)の高いものが提案されている。(特開昭53
−4059)。そこで硬度あいいは複素弾性率の高い
加硫ゴムを作成する方法として熱硬化性レジンあ
るいはカーボンの配合量を増加させるか、あるい
は硫黄、加硫促進剤を多量使用し架橋密度を増加
させることが行われている。しかし前者はバンバ
リーミキサーでゴムを混練する際、発熱性が高
く、そのためゴムがスコーチしてしまつたり、ま
た組成物自体の粘度が高いため混練、押し出しの
際過度の負荷を発生する。また後者は組成物を加
工する際、硫黄がブルーミングしてゴムの粘着性
を損なうほか、加硫ゴム物性を低下させる問題が
ある。本発明はこれらの問題点を解決することを
目的とするものであり、作業性等の問題なく極め
て硬度の高いゴム組成物を提案するものである。
本発明は少なくとも1種類のジエン系ゴム100
重量部に芳香族ポリアミドパルプの直径0.1〜1μ、
長さ3〜1000μのフイブリル1〜30重量部、熱硬
化性樹脂を2〜40重量部、硬化剤を1〜20重量部
配合したことを特徴とするビードエイペツクス用
硬質ゴム組成物である。
本発明で用いられる芳香族ポリアミドパルプは
芳香族ポリアミド繊維から製造できるほか、芳香
族ポリアミドポリマーを合成する段階で製造する
ことができるが、このパルプは直径0.1〜1μ、長
さ3〜1000μのフイブリルを有する。この芳香族
ポリアミドパルプは微細分枝を有するため、ゴム
中に混練することによりゴムと分子レベルでの混
合が可能となり繊維コードあるいは短繊維を混合
する場合よりも、より効果的な補強が達成でき
る。直径が0.1μ未満の場合及び長さが3μ未満の場
合には、ゴムへの配合が困難となり、またビード
エイペツクスに用いたとき必要な剛性を確保する
ことができない。また、直径が1μを越えた場合、
及び長さが1000μを越えた場合にはゴム中の分散
不良を生じる。
なお芳香族ポリアミドパルプは1〜30重量部、
好ましくは5〜20重量部配合することが必要であ
り、1重量部より少ないと補強効果は充分でなく
作業性が悪くなる。
次に本発明では熱硬化性樹脂及び硬化剤を配合
することを必要とする。ここで熱硬化性樹脂とは
フエノール樹脂、クレゾール樹脂、もしくはこれ
らの変性樹脂、例えばカシユーワニス変性樹脂、
リノール酸、リノレン酸、オレイン酸等のオイル
で変性したオイル変性樹脂、キシレン等のアルキ
ルベンゼンで変性したアルキルベンゼン変性フエ
ノール、エポキシ変性樹脂、アニリン変性樹脂、
メラミン変性樹脂等の熱によつて硬化する樹脂で
単独もしくは二種類以上を任意の割合に混合して
用いられる。この熱硬化性樹脂はゴム成分100重
量部に対して2〜40重量部、好ましくは10〜20重
量部配合される。2重量部より少ないと補強効果
は充分でなく、また40重量部を越えると混練作業
性が著しく阻害される。
次に本発明で使用される硬化剤は前記熱硬化性
樹脂を硬化させるもので、40〜200℃、特に通常
の加硫条件下で加硫したばあいメチレン基を供与
する化合物、所謂メチレン供与体である。例えば
ヘキサメチレンテトラミン、多価メチロールメラ
ミン誘導体、オキサゾリジン、ビス(1,3オキ
サゾリジン)、ビス(1,3オキサゾリジン)誘
導体等である。なおこの硬化剤の配合量は熱硬化
性樹脂の配合量に応じて調整する必要があるがゴ
ム成分100重量部に対して0.5〜7重量部配合され
る。なお熱硬化性樹脂及び硬化剤を前記芳香族ポ
リアミドパルプと併用することにより加硫ゴムの
硬度及び複素弾性率を一層高めることができる。
なお本発明で用いられるジエン系ゴムは天然ゴ
ム、シス1,4ポリイソプレンゴムイ、シス1,
4ポリブタジエンゴム、スチレンーブタジエン共
重合ゴム等を単独または二種類以上をブレンドで
用いることができる。更に本発明の組成物は通常
用いられる配合剤、例えばカーボン、シリカ等の
充填剤のほか軟化剤、老化防止剤、加硫促進剤、
可塑剤等を適宜配合できることは勿論である。
然して本発明に係るゴム組成物を常法により加
硫することにより耐屈曲亀裂性、低発熱性、高い
硬度等の特性を維持しながら混練作業性、押し出
し加工性等の特性を一層改善することが可能とな
る。
実施例 1
第1表に示す各種のビードエーペツクス用ゴム
配合について150℃で30分加硫ち、そのモジユラ
ス、硬度、複素弾性率等を測定し、その結果を第
2表に示す。芳香族ポリアミドパルプとフエノー
ル樹脂の併用によつて向上することが認められ
る。
The present invention relates to a hard rubber composition, particularly a hard rubber composition suitable for bead apex or clinch apex. The present invention relates to a hard rubber composition containing a curing agent. Generally, in radial tires, the carcass ply cords are arranged parallel to each other at almost right angles to the tire equatorial plane, and both ends are folded back around the bead wire, and the folded ends of the ply and the inner side surrounded by the carcass are Bead apexes are disposed extending in the direction of the wall, and clinch apexes are disposed in areas adjacent to the rim flange at the outer ends of the folds of the plies. Tires with a radial structure like this have a step in stiffness at the folded end of the ply, which is prone to damage, and because it is a radial structure, it inherently has poor lateral stiffness. Bead apexes or clinch apex having particularly high hardness (or dynamic elastic modulus) have been proposed. (Unexamined Japanese Patent Publication 1973)
−4059). Therefore, in order to create a vulcanized rubber with a high complex modulus, it is possible to increase the hardness by increasing the amount of thermosetting resin or carbon, or by using large amounts of sulfur or vulcanization accelerators to increase the crosslinking density. It is being done. However, when the former rubber is kneaded in a Banbury mixer, it generates a lot of heat, which causes the rubber to scorch, and the composition itself has a high viscosity, which causes an excessive load during kneading and extrusion. In addition, the latter has the problem that sulfur blooms during processing of the composition, impairing the tackiness of the rubber and deteriorating the physical properties of the vulcanized rubber. The present invention aims to solve these problems, and proposes a rubber composition that has extremely high hardness without problems such as workability. The present invention provides at least one diene rubber 100
Aromatic polyamide pulp diameter 0.1~1μ in weight part,
A hard rubber composition for bead apex comprising 1 to 30 parts by weight of fibrils having a length of 3 to 1000 μ, 2 to 40 parts by weight of a thermosetting resin, and 1 to 20 parts by weight of a curing agent. . The aromatic polyamide pulp used in the present invention can be manufactured from aromatic polyamide fibers, or can be manufactured at the stage of synthesizing aromatic polyamide polymer, but this pulp consists of fibrils with a diameter of 0.1 to 1 μm and a length of 3 to 1000 μm. has. Since this aromatic polyamide pulp has fine branches, it can be mixed with rubber at the molecular level by kneading it into rubber, achieving more effective reinforcement than when mixing fiber cords or short fibers. . If the diameter is less than 0.1μ or the length is less than 3μ, it will be difficult to incorporate into rubber, and it will not be possible to secure the necessary rigidity when used in bead apex. In addition, if the diameter exceeds 1μ,
If the length exceeds 1000μ, poor dispersion in the rubber will occur. In addition, the aromatic polyamide pulp is 1 to 30 parts by weight,
Preferably, it is necessary to mix 5 to 20 parts by weight, and if it is less than 1 part by weight, the reinforcing effect will not be sufficient and workability will deteriorate. Next, the present invention requires blending a thermosetting resin and a curing agent. Here, thermosetting resins include phenolic resins, cresol resins, or modified resins thereof, such as cashew varnish modified resins,
Oil-modified resins modified with oils such as linoleic acid, linolenic acid, and oleic acid, alkylbenzene-modified phenols modified with alkylbenzenes such as xylene, epoxy-modified resins, aniline-modified resins,
Resins that harden by heat, such as melamine-modified resins, can be used alone or in combination of two or more in any proportion. This thermosetting resin is blended in an amount of 2 to 40 parts by weight, preferably 10 to 20 parts by weight, per 100 parts by weight of the rubber component. If it is less than 2 parts by weight, the reinforcing effect will not be sufficient, and if it exceeds 40 parts by weight, the kneading workability will be significantly impaired. Next, the curing agent used in the present invention is one that cures the thermosetting resin, and is a compound that donates methylene groups when vulcanized at 40 to 200°C, especially under normal vulcanization conditions, so-called methylene donor. It is the body. Examples include hexamethylenetetramine, polyvalent methylolmelamine derivatives, oxazolidine, bis(1,3 oxazolidine), bis(1,3 oxazolidine) derivatives, and the like. The amount of this curing agent needs to be adjusted depending on the amount of thermosetting resin, but it is blended in an amount of 0.5 to 7 parts by weight per 100 parts by weight of the rubber component. Note that by using a thermosetting resin and a curing agent together with the aromatic polyamide pulp, the hardness and complex modulus of the vulcanized rubber can be further increased. The diene rubber used in the present invention includes natural rubber, cis 1,4 polyisoprene rubber, cis 1,
4-polybutadiene rubber, styrene-butadiene copolymer rubber, etc. can be used alone or in a blend of two or more. Furthermore, the composition of the present invention contains commonly used compounding agents, such as fillers such as carbon and silica, as well as softeners, anti-aging agents, vulcanization accelerators,
It goes without saying that plasticizers and the like can be added as appropriate. However, by vulcanizing the rubber composition according to the present invention by a conventional method, properties such as kneading workability and extrusion processability can be further improved while maintaining properties such as flex crack resistance, low heat build-up, and high hardness. becomes possible. Example 1 The various rubber formulations for bead apex shown in Table 1 were vulcanized at 150°C for 30 minutes, and their modulus, hardness, complex modulus, etc. were measured, and the results are shown in Table 2. It is recognized that the use of aromatic polyamide pulp and phenolic resin in combination improves the performance.
【表】【table】
【表】【table】
Claims (1)
に芳香族ポリアミドパルプの直径0.1〜1μ、長さ
3〜1000μのフイブリル1〜30重量部、熱硬化性
樹脂を2〜40重量部、硬化剤を1〜20重量部配合
したことを特徴とするビードエイペツクス用硬質
ゴム組成物。 2 熱硬化性樹脂はフエノール樹脂、クレゾール
樹脂もしくは変性樹脂であることを特徴とする特
許請求の範囲第1項記載のビードエイペツクス用
硬質ゴム組成物。 3 硬化剤はオキサゾリジン誘導体である特許請
求の範囲第1項記載の硬質ゴム組成物。 4 硬化剤はヘキサメチレンテトラミンである特
許請求の範囲第1項記載の硬質ゴム組成物。[Claims] 1. 100 parts by weight of at least one type of diene rubber, 1 to 30 parts by weight of aromatic polyamide pulp fibrils having a diameter of 0.1 to 1 μm and a length of 3 to 1000 μm, and 2 to 40 parts by weight of a thermosetting resin. A hard rubber composition for bead apex, characterized in that it contains 1 to 20 parts by weight of a curing agent. 2. The hard rubber composition for bead apex according to claim 1, wherein the thermosetting resin is a phenolic resin, a cresol resin, or a modified resin. 3. The hard rubber composition according to claim 1, wherein the curing agent is an oxazolidine derivative. 4. The hard rubber composition according to claim 1, wherein the curing agent is hexamethylenetetramine.
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
JP1272037A JPH0328243A (en) | 1989-10-18 | 1989-10-18 | Hard rubber composition |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
JP1272037A JPH0328243A (en) | 1989-10-18 | 1989-10-18 | Hard rubber composition |
Related Parent Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
JP7416782A Division JPS58189244A (en) | 1982-04-30 | 1982-04-30 | Hard rubber composition |
Publications (2)
Publication Number | Publication Date |
---|---|
JPH0328243A JPH0328243A (en) | 1991-02-06 |
JPH04100B2 true JPH04100B2 (en) | 1992-01-06 |
Family
ID=17508245
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
JP1272037A Granted JPH0328243A (en) | 1989-10-18 | 1989-10-18 | Hard rubber composition |
Country Status (1)
Country | Link |
---|---|
JP (1) | JPH0328243A (en) |
Families Citing this family (12)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CA2079522A1 (en) * | 1991-09-30 | 1993-03-31 | Yukishige Adachi | Pneumatic radial tire |
US5885389A (en) * | 1997-03-06 | 1999-03-23 | The Goodyear Tire & Rubber Company | Tire with chafer composition |
JP3090444B2 (en) * | 1998-06-19 | 2000-09-18 | 住友ゴム工業株式会社 | Pneumatic tire |
WO2002078983A1 (en) * | 2001-03-30 | 2002-10-10 | Pirelli Pneumatici S.P.A. | Tyre for vehicle wheels with a reinforced bead |
JP4478375B2 (en) * | 2002-08-20 | 2010-06-09 | 株式会社ブリヂストン | tire |
US7317063B2 (en) * | 2003-03-07 | 2008-01-08 | Angus Chemical Company | Phenolic resins |
US20040116647A1 (en) * | 2002-12-04 | 2004-06-17 | Swedo Raymond J. | Novel phenolic resins |
US7015274B2 (en) | 2003-05-02 | 2006-03-21 | E. I. Du Pont De Nemours And Company | Polymer precursor dispersion containing a micropulp and method of making the dispersion |
JP2007112834A (en) * | 2005-10-18 | 2007-05-10 | Sumitomo Rubber Ind Ltd | Rubber composition for tire and pneumatic tire by using the same |
JP4884316B2 (en) * | 2006-07-11 | 2012-02-29 | 住友ゴム工業株式会社 | Rubber composition for bead apex and tire having bead apex using the same |
WO2008007562A1 (en) | 2006-07-11 | 2008-01-17 | Sumitomo Rubber Industries, Ltd. | Rubber composition for bead apex and tire with bead apex utilizing the same |
JP4724691B2 (en) * | 2007-06-19 | 2011-07-13 | 株式会社オーティス | Pipe mounting structure |
-
1989
- 1989-10-18 JP JP1272037A patent/JPH0328243A/en active Granted
Also Published As
Publication number | Publication date |
---|---|
JPH0328243A (en) | 1991-02-06 |
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