JPH0615637B2 - Rubber compounding composition for tire tread - Google Patents
Rubber compounding composition for tire treadInfo
- Publication number
- JPH0615637B2 JPH0615637B2 JP60157680A JP15768085A JPH0615637B2 JP H0615637 B2 JPH0615637 B2 JP H0615637B2 JP 60157680 A JP60157680 A JP 60157680A JP 15768085 A JP15768085 A JP 15768085A JP H0615637 B2 JPH0615637 B2 JP H0615637B2
- Authority
- JP
- Japan
- Prior art keywords
- rubber
- parts
- weight
- composition
- copolymer
- 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
- B60—VEHICLES IN GENERAL
- B60C—VEHICLE TYRES; TYRE INFLATION; TYRE CHANGING; CONNECTING VALVES TO INFLATABLE ELASTIC BODIES IN GENERAL; DEVICES OR ARRANGEMENTS RELATED TO TYRES
- B60C1/00—Tyres characterised by the chemical composition or the physical arrangement or mixture of the composition
- B60C1/0016—Compositions of the tread
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L21/00—Compositions of unspecified rubbers
Landscapes
- Chemical & Material Sciences (AREA)
- Health & Medical Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Medicinal Chemistry (AREA)
- Polymers & Plastics (AREA)
- Organic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Mechanical Engineering (AREA)
- Compositions Of Macromolecular Compounds (AREA)
- Tires In General (AREA)
Description
【発明の詳細な説明】 （産業上の利用分野） 本発明は炭素数４〜５の脂肪族オレフイン・ジオレフイ
ンと炭素数９〜10の芳香族オレフインの共重合体が添加
されたタイヤトレツド用ゴム配合組成物に関するもので
あり、走行時における操縦安定性、晴・雨天時の制動性
を飛躍的に向上させ、且つ従来の問題点であつた耐チツ
ピング、耐クラツク性も向上させたタイヤトレツド用ゴ
ム配合組成物に関するものである。DETAILED DESCRIPTION OF THE INVENTION (Industrial field of application) The present invention relates to a rubber compound for tire tires to which a copolymer of an aliphatic olefin / diolephine having 4 to 5 carbon atoms and an aromatic olefin having 9 to 10 carbon atoms is added. A rubber compound for tire tires that is related to a composition and has drastically improved steering stability during driving, braking performance in fine weather and rain, and improved chipping resistance and cracking resistance, which have been problems in the past. It relates to a composition.
（従来の技術） 近年、自動車の高馬力化、軽量化に伴ない、タイヤに要
求される性能としては、操縦安定性と制動性に対してよ
り厳しい要望が求められている。とりわけ、車の走行時
におけるレーン変更等におけるハンドルの応答性や雨天
時における制動性能が重要であり、これらの性能を向上
させたタイヤが要求されている。(Prior Art) With the recent trend toward higher horsepower and lighter weight of automobiles, stricter demands on steering stability and braking performance are required as performances required for tires. In particular, the responsiveness of the steering wheel when changing the lane when the vehicle is running and the braking performance in rainy weather are important, and tires with improved performance are required.
これらの要求を満たすためには、トレツドゴムの摩擦係
数を大きくし、かつＷet Ｓkid性を改善することが必
要である。従来、トレツドゴムの摩擦係数を大きくし、
かつＷet Ｓkid性を改善する方法としては、カーボ
ンブラツク及びオイルの多量使用、スチレン含有量の
多いスチレン・ブタジエン共重合体の利用、樹脂の利
用等が一般に知られている。また、特開昭55−110136、
56−163907号にはニトリルゴム使用して制動性を改良す
る方法が記載されている。しかし、これらの方法はいず
れもトラツク特性の低下、発熱特性の低下を伴い、さら
に、極性の小さいゴムにニトリルゴムをブレンドした場
合には、両者は極性が異なるので均一に相溶せず無極性
ゴム中に極性ゴムが微小粒子になつて散在しクラツク特
性、チツピング特性、摩耗特性を低下させ、トレツドゴ
ム組成物として使用した場合、タイヤの製品寿命に悪影
響を及ぼすので好ましくない。In order to meet these requirements, it is necessary to increase the friction coefficient of the tread rubber and improve the wet skid property. Conventionally, the friction coefficient of the tread rubber has been increased,
In addition, as a method for improving the wet skid property, the use of a large amount of carbon black and oil, the use of a styrene-butadiene copolymer having a high styrene content, the use of a resin, etc. are generally known. Further, JP-A-55-110136,
56-163907 describes the use of nitrile rubber to improve braking. However, all of these methods are accompanied by a decrease in track characteristics and a decrease in heat generation characteristics.In addition, when a nitrile rubber is blended with a rubber having a small polarity, the two polarities are different from each other and are not compatible with each other. Polar rubber is dispersed in the rubber in the form of fine particles to deteriorate cracking properties, chipping properties, and wear properties, and when it is used as a tread rubber composition, it adversely affects the product life of the tire, which is not preferable.
（発明が解決しようとする問題点） 本発明の目的は、トレツドゴム配合組成物が高い摩擦係
数をもち、Ｗet Ｓkid性も高いと同時に、クラツク特
性及び発熱特性の低下を引き起こさない組成物を提供す
ることにある。(Problems to be Solved by the Invention) An object of the present invention is to provide a composition having a high friction coefficient and a high wet skid property, and at the same time, not causing a decrease in crack characteristics and exothermic characteristics. Especially.
（問題点を解決するための手段） 本発明はゴム成分100重量部に対し、炭素数４〜５の脂
肪族オレフイン・ジオレフインと炭素数９〜10の芳香族
オレフインの共重合体２〜30重量部、Ｎ2ＳＡが902/g以
上のフアーネスカーボン60〜110重量部を含有するタイ
ヤトレツド用ゴム配合組成物に係る。(Means for Solving Problems) The present invention is based on 100 parts by weight of a rubber component, and 2 to 30 parts by weight of a copolymer of an aliphatic olefin / diolephine having 4 to 5 carbon atoms and an aromatic olephine having 9 to 10 carbon atoms. Part, and a rubber compounding composition for a tire tread containing 60 to 110 parts by weight of furnace carbon having N 2 SA of 90 2 / g or more.
本発明においてゴム成分としては天然ゴム(ＮＲ)及び合
成ゴムの１種又は２種以上が用いられる。合成ゴムとし
ては例えばポリイソプレンゴム(ＩＲ)、ポリブタジエン
ゴム(ＢＲ)、スチレン・ブタジエンゴム(ＳＢＲ)、イソ
プレン・イソブチレンゴム(ＩＩＲ)、エチレン・プロピ
レン・ジエンゴム(ＥＰＤＭ)、これらの変性物、これら
のブレンド物等がいずれも使用できる。In the present invention, as the rubber component, one type or two or more types of natural rubber (NR) and synthetic rubber are used. Examples of synthetic rubber include polyisoprene rubber (IR), polybutadiene rubber (BR), styrene-butadiene rubber (SBR), isoprene-isobutylene rubber (IIR), ethylene-propylene-diene rubber (EPDM), modified products thereof, and modified products thereof. Any of blended materials and the like can be used.
本発明で使用する炭素数４〜５の脂肪族オレフイン・ジ
オレフインと炭素数９〜10の芳香族オレフインの共重合
体（以下、ＡＡ共重合体という)において、炭素数４〜
５の脂肪族オレフイン・ジオレフインとしてはブテン、
イソブテン、ペンテン、メチルブテン、ブタジエン、ペ
ンタジエンなどを、また炭素数９〜10の芳香族オレフイ
ンとしてはα−メチルスチレン、β−メチルスチレン、
２−フエニル−２−ブテン、１−フエニル−１−ブテ
ン、３−フエニル−１−ブテン、１−フエニル−1,3−
ブタジエン、ジビニルベンゼン、フエニルアレン、２−
フエニル−1,3−ブタジエンなどを挙げることができ、
これらは単独で又は２種以上の混合物として用いること
ができる。ＡＡ共重合体の重量平均分子量は特に500〜1
000の範囲が好ましい。またJIS K2207により測定した
軟化点が80〜120℃、より好ましくは95〜105℃の範囲が
良い。ＡＡ共重合体の配合量はゴム成分100部(重量部、
以下同様)に対して２〜30部が好適である。２部未満で
は十分な効果が達成されず、30部を越える場合はロール
やバンバリーミキサーのローターへ過粘着することがあ
り加工性で問題を生じやすい。In the copolymer of the aliphatic olefin / diorefin having 4 to 5 carbon atoms and the aromatic olefin having 9 to 10 carbon atoms (hereinafter referred to as AA copolymer) used in the present invention, the number of carbon atoms of 4 to
Butene as an aliphatic olefin / diorefin of 5,
Isobutene, pentene, methylbutene, butadiene, pentadiene and the like, and as aromatic olefins having 9 to 10 carbon atoms, α-methylstyrene, β-methylstyrene,
2-phenyl-2-butene, 1-phenyl-1-butene, 3-phenyl-1-butene, 1-phenyl-1,3-
Butadiene, divinylbenzene, phenylarene, 2-
Examples include phenyl-1,3-butadiene,
These can be used alone or as a mixture of two or more kinds. The weight average molecular weight of the AA copolymer is especially 500 to 1
A range of 000 is preferred. The softening point measured according to JIS K2207 is preferably 80 to 120 ° C, more preferably 95 to 105 ° C. The compounding amount of the AA copolymer is 100 parts by weight of the rubber component (parts by weight,
2 to 30 parts are preferable for the same). If it is less than 2 parts, a sufficient effect cannot be achieved, and if it exceeds 30 parts, it may be excessively adhered to a roll or a rotor of a Banbury mixer, which may cause a problem in processability.
本発明で使用するフアーネスカーボンはASTM Ｄ3037の
窒素吸着法による比表面積(Ｎ2ＳＡ)が90m2/g以上のも
のであり、Ｎ2ＳＡが90m2/g未満では高い摩擦係数を維
持することができず、耐摩耗性も劣ってくる。フアーネ
スカーボンの配合量はゴム成分100重量部に対して60〜1
10重量部が好適である。The furnace carbon used in the present invention has a specific surface area (N 2 SA) of 90 m 2 / g or more according to the nitrogen adsorption method of ASTM D3037, and maintains a high friction coefficient when N 2 SA is less than 90 m 2 / g. It is not possible, and wear resistance becomes poor. The amount of furnace carbon is 60 to 1 per 100 parts by weight of the rubber component.
10 parts by weight is preferred.
本発明のゴム組成物は上記成分を通常の加工装置、例え
ばロール、バンバリーミキサー、ニーダーなどにより混
練することにより得られる。また上記成分の他に公知の
加硫剤、加硫促進剤、加硫促進助剤、加硫遅延剤、有機
過酸化物、補強剤、充填剤、老化防止剤、粘着付与剤、
着色剤等を添加できることは勿論である。The rubber composition of the present invention can be obtained by kneading the above components with a conventional processing device such as a roll, a Banbury mixer or a kneader. In addition to the above components, known vulcanizing agents, vulcanization accelerators, vulcanization accelerating aids, vulcanization retarders, organic peroxides, reinforcing agents, fillers, antioxidants, tackifiers,
Of course, a colorant or the like can be added.
（実施例） 以下に実施例及び比較例により詳細に説明する。(Example) Below, it demonstrates in detail by an Example and a comparative example.
硬度特性(Ｈｓs)はJIS Ｋ6301に従つて測定し、摩擦係
数はポータブルスキツドテスターを用いてアスフアルト
路面上で測定し、比較例１をコントロールとしてインデ
ツクス表示(μインデツクスとして示す)した。値の大き
いもの程、良好である。The hardness characteristics (Hss) were measured according to JIS K6301, and the friction coefficient was measured on an asphalt road surface using a portable skid tester, and Comparative Example 1 was used as a control for index display (shown as μ index). The larger the value, the better.
耐クラツク性は、デマーチヤ試験機を用い、300サイク
ル／分、40℃にて、試験片0.5×2.5×30mmを歪100％の
条件下で伸張歪を与え、ワイブル確率50％になるまでの
サイクル数を比較例１を100として指数を表わす。値の
大きいものほど良好である。発熱度はグツドリツチフレ
クソメーターにてストローク４．４mm、荷重10.9kg、振
動数1800rpm、初期温度40℃の条件で25分間振動した後
のゴムの表面温度を測定し初期温度40をマイナスした値
で示す。The crack resistance is a cycle until a Weibull probability of 50% is reached by applying a tensile strain to a test piece of 0.5 × 2.5 × 30 mm at a strain of 100% at 300 cycles / min at 40 ° C. using a demarcher tester. The index is expressed by setting the number to 100 in Comparative Example 1. The larger the value, the better. The degree of heat generation was measured by measuring the surface temperature of the rubber after vibrating for 25 minutes under the conditions of a stroke of 4.4 mm, a load of 10.9 kg, a frequency of 1800 rpm, and an initial temperature of 40 ° C. using a guddrichch flexometer, and the initial temperature of 40 was subtracted. Indicated by value.
実施例１〜６及び比較例１〜10 第１表に記載の割合のゴム成分、カーボンブラツク、ア
ロマテイツクオイル、各種樹脂に、亜鉛華３部、ステア
リン酸２部、老化防止剤(パラフエニレンジアミン系)１
部、加硫促進剤(チアゾール系)１部、加硫促進剤(グア
ニジン系)０．４部及び硫黄２部をバンバリーミキサー
により均一に混練してゴム組成物を得た。各ゴム組成物
の物性も第１表に示す。尚、表において、 (１)は23.5％スチレン含量のＥ−ＳＢＲ (２)は40％スチレン含量のＥ−ＳＢＲ (３)は25％スチレン含量のＥ−ＳＢＲ (４)はＮ2ＳＡ93，ＤＢＰ120のフアーネスカーボン (５)はＮ2ＳＡ113，ＤＢＰ114のフアーネスカーボン (６)はＮ2ＳＡ72，ＤＢＰ120のフアーネスカーボン (７)はテルペンフエノール系樹脂、Ｔs＝145℃ (８)は脂肪族系樹脂、Ｔs＝145℃ (９)はアルキルフエノール樹脂、Ｔs＝70〜85℃ (10) 芳香族系炭化水素樹脂、Ｔs＝130℃ (11) は三井石油化学製のＡＡ共重合体で商品名Ｔack
Ａce Ａ−100 尚、上記でＥ−ＳＢＲは乳化重合ＳＢＲ、Ｓ−ＳＢＲは
溶液重合ＳＢＲ、ＤＢＰはジブチルフタレート吸収量を
示す。Examples 1 to 6 and Comparative Examples 1 to 10 Rubber component, carbon black, aromatic oil, and various resins in the proportions shown in Table 1 were added to 3 parts of zinc white, 2 parts of stearic acid, an antioxidant (paraphenylene). (Diamine type) 1
Parts, 1 part of vulcanization accelerator (thiazole type), 0.4 parts of vulcanization accelerator (guanidine type) and 2 parts of sulfur were uniformly kneaded with a Banbury mixer to obtain a rubber composition. The physical properties of each rubber composition are also shown in Table 1. In the table, (1) is E-SBR having 23.5% styrene content (2) is E-SBR having 40% styrene content (3) is E-SBR having 25% styrene content (4) is N 2 SA93, DBP120 of fir Ness carbon (5) is N 2 SA113, DBP114 Sulfur Ness carbon (6) is N 2 SA72, DBP120 Sulfur Ness carbon (7) of the terpene phenol resin, Ts = 145 ℃ (8) of the aliphatic Resin, Ts = 145 ° C (9) is an alkylphenol resin, Ts = 70 to 85 ° C (10) Aromatic hydrocarbon resin, Ts = 130 ° C (11) is an AA copolymer manufactured by Mitsui Petrochemical Co., Ltd. Tack
Ace A-100 In the above, E-SBR indicates emulsion polymerization SBR, S-SBR indicates solution polymerization SBR, and DBP indicates dibutyl phthalate absorption amount.
試験例１ 実施例及び比較例の配合組成物をトレツドに用いて、タ
イヤサイズ175/70ＨＲ13なる乗用車用ラジアルタイヤを
試作し、タイヤの制動性、操縦安定性、チツピング性を
評価した。結果を第２表に示す。Test Example 1 A radial tire for passenger cars having a tire size of 175 / 70HR13 was prototyped using the compounded compositions of Examples and Comparative Examples in a tread, and the braking performance, steering stability, and chipping performance of the tire were evaluated. The results are shown in Table 2.
タイヤのＤry、Ｗet制動は荷重336kg、空気圧1.8kg/cm2
の条件で米国のＬＴＱＧＳに定められた方法で測定し、
比較例１をコントロールとしてインデツクス表示する。
値の大きい程、良好である。Dry and Wet braking of tires has a load of 336kg and air pressure of 1.8kg / cm 2.
Measured by the method specified in the US LTQGS under the conditions of
An index is displayed using Comparative Example 1 as a control.
The larger the value, the better.
操縦安定性は荷重400kgでコーナリングパワーを測定
し、比較例１をコントロールとしてインデツクス表示す
る。値の大きい程、良好である。The steering stability is measured by measuring the cornering power with a load of 400 kg and displaying the index by using Comparative Example 1 as a control. The larger the value, the better.
耐チツピング特性は極悪路2500kmを走行させた後のトレ
ツド外観を観察し、比較例１を３として５段階の相対評
価を行つた。５は優、１は劣である。Regarding the chipping resistance, the appearance of the tread after traveling 2500 km on a terrible road was observed, and the relative evaluation was carried out in five stages with Comparative Example 1 as 3. 5 is excellent and 1 is inferior.
（発明の効果） 第１表において、実施例１及び２は、ＡＡ共重合体を添
加又はプロセスオイルと置換することにより、比較例１
に比べ発熱性は殆ど変化なく、μインデツクスが向上
し、耐クラツク特性も向上している。 (Effect of the invention) In Table 1, in Examples 1 and 2, Comparative Example 1 was prepared by adding the AA copolymer or replacing it with the process oil.
Compared to the above, the heat generation property is almost unchanged, the μ index is improved, and the crack resistance property is also improved.
比較例２のμインデツクスの向上を図つたものが、比較
例５〜９であり、スチレン含有量の多いＳＢＲの利用、
樹脂の利用によりμインデツクスは向上しているが、耐
クラツク性や発熱性が低下している。Comparative Examples 2 to 9 aim to improve the μ index of Comparative Example 2 and use SBR having a high styrene content,
Although the μ index is improved by using the resin, the crack resistance and heat generation property are deteriorated.
比較例３はカーボンの配合量が60部未満の例であり、μ
インデツクスが維持できない。又、比較例４はＮ2ＳＡ
が90未満のカーボンを使用した場合で、実施例１や比較
例１に比べてもμインデツクスは低下している。比較例
10は比較例１に対して、耐クラツク特性を向上させたも
のだが、μインデツクスが劣つていて、実施例１の方が
耐クラツク特性も向上している。Comparative Example 3 is an example in which the amount of carbon blended is less than 60 parts.
The index cannot be maintained. In addition, Comparative Example 4 is N 2 SA
In the case of using a carbon of less than 90, the μ index is lower than that of Example 1 and Comparative Example 1. Comparative example
Although 10 has improved cracking resistance as compared with Comparative Example 1, the μ index is inferior, and Example 1 also has improved cracking resistance.
第２表より、本発明の組成物は高い制動性能とコーナリ
ング安定性をもち、チツピング特性も良好であることが
明らかである。From Table 2, it is clear that the composition of the present invention has high braking performance and cornering stability, and good chipping characteristics.
Claims (2)
ジエンゴム、スチレン・ブタジエンゴム、イソプレン・
イソブチレンゴム、エチレン・プロピレン・ジエンゴム
及びこれらの変性物の群から選ばれた１種又は２種以上
のゴム成分100重量部に対し、炭素数４〜５の脂肪族オ
レフイン・ジオレフインと炭素数９〜10の芳香族オレフ
インの共重合体２〜30重量部、Ｎ2ＳＡが90m2／g以上の
フアーネスカーボン60〜110重量部を含有するタイヤト
レツド用ゴム配合組成物。1. Natural rubber, polyisoprene rubber, polybutadiene rubber, styrene-butadiene rubber, isoprene
100 parts by weight of one or two or more rubber components selected from the group consisting of isobutylene rubber, ethylene / propylene / diene rubber and modified products thereof, and aliphatic olefin / diolephine having 4 to 5 carbon atoms and 9 to 9 carbon atoms A rubber compounding composition for a tire tread, containing 2 to 30 parts by weight of a copolymer of 10 aromatic olefins and 60 to 110 parts by weight of furnace carbon having N 2 SA of 90 m 2 / g or more.
0である特許請求の範囲第１項記載の組成物。2. The copolymer has a weight average molecular weight of 500 to 100.
The composition of claim 1 wherein the composition is 0.
Priority Applications (3)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP60157680A JPH0615637B2 (en) | 1985-07-17 | 1985-07-17 | Rubber compounding composition for tire tread |
| GB08617247A GB2178046B (en) | 1985-07-17 | 1986-07-15 | Rubber composition for tyre treads |
| DE19863624221 DE3624221C1 (en) | 1985-07-17 | 1986-07-17 | Rubber composition for tire treads |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP60157680A JPH0615637B2 (en) | 1985-07-17 | 1985-07-17 | Rubber compounding composition for tire tread |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS6218447A JPS6218447A (en) | 1987-01-27 |
| JPH0615637B2 true JPH0615637B2 (en) | 1994-03-02 |
Family
ID=15655036
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP60157680A Expired - Lifetime JPH0615637B2 (en) | 1985-07-17 | 1985-07-17 | Rubber compounding composition for tire tread |
Country Status (3)
| Country | Link |
|---|---|
| JP (1) | JPH0615637B2 (en) |
| DE (1) | DE3624221C1 (en) |
| GB (1) | GB2178046B (en) |
Families Citing this family (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CA1319091C (en) * | 1987-09-03 | 1993-06-15 | Seiichiro Iwafune | Pneumatic tires |
| JPH0539916U (en) * | 1992-10-12 | 1993-05-28 | 大豊精機株式会社 | Screw conveyor type conveyor |
| EP0697432B1 (en) * | 1994-08-19 | 2003-10-15 | Bridgestone Corporation | Rubber composition for tire treads |
| FR2910905B1 (en) | 2006-12-27 | 2010-08-20 | Michelin Soc Tech | PLASTICATING SYSTEM AND RUBBER COMPOSITION FOR PNEUMATIC INCORPORATING SAID SYSTEM |
| JP6843656B2 (en) * | 2017-03-10 | 2021-03-17 | 大塚化学株式会社 | Rubber composition with excellent tear strength |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS4838338A (en) * | 1971-09-17 | 1973-06-06 | ||
| JPS59140241A (en) * | 1983-01-31 | 1984-08-11 | Tokai Carbon Co Ltd | Rubber composition |
-
1985
- 1985-07-17 JP JP60157680A patent/JPH0615637B2/en not_active Expired - Lifetime
-
1986
- 1986-07-15 GB GB08617247A patent/GB2178046B/en not_active Expired
- 1986-07-17 DE DE19863624221 patent/DE3624221C1/en not_active Expired
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS4838338A (en) * | 1971-09-17 | 1973-06-06 | ||
| JPS59140241A (en) * | 1983-01-31 | 1984-08-11 | Tokai Carbon Co Ltd | Rubber composition |
Also Published As
| Publication number | Publication date |
|---|---|
| GB2178046A (en) | 1987-02-04 |
| GB8617247D0 (en) | 1986-08-20 |
| DE3624221C1 (en) | 1987-03-12 |
| JPS6218447A (en) | 1987-01-27 |
| GB2178046B (en) | 1988-10-26 |
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Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| EXPY | Cancellation because of completion of term |