JPS6158506B2 - - Google Patents
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- Publication number
- JPS6158506B2 JPS6158506B2 JP52057387A JP5738777A JPS6158506B2 JP S6158506 B2 JPS6158506 B2 JP S6158506B2 JP 52057387 A JP52057387 A JP 52057387A JP 5738777 A JP5738777 A JP 5738777A JP S6158506 B2 JPS6158506 B2 JP S6158506B2
- Authority
- JP
- Japan
- Prior art keywords
- sensitive adhesive
- pressure
- heating
- adhesive material
- weight
- 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
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- Lining Or Joining Of Plastics Or The Like (AREA)
- Adhesive Tapes (AREA)
- Adhesives Or Adhesive Processes (AREA)
Description
この発明は、電気装置、機械装置、住設機器な
どの物品あるいはコンクリート面、壁面などの構
造物の表面(以下基礎面という)に、銘板、小物
品などの貼り付け物品を貼り付ける新規な貼り付
け方法に関する。
この発明は、基礎面に、常態においては基礎面
に貼り付け物品を仮止め出来る程度の弱い接着性
を有し、且つ約90℃以下の比較的低い加熱で短時
間加熱することにより熱感応して通常知られる感
圧性接着剤の常温におけると同等の弾性率を有す
る粘度に活性化されて十分な接着強度を発揮する
特定の熱時感圧性接着材料を介して貼り付け物品
を重ね合わせ、然る後加熱または加熱加圧するこ
とによつて、室温状態あるいは加熱状態下の使用
で強い接着状態が維持される貼り付け方法を提供
するものである。
従来、銘板、パンチングプレート、装飾板の如
き表面板あるいは貼着懸垂具、パネルなどの小物
品などの貼り付け物品を基礎面に貼り付けるに際
しては、支持体面に感圧性接着剤を形成してなる
所謂両面感圧性接着テープが用いられている。し
かして該接着剤を用いてなるテープを用いて、基
礎面に貼り付け物品を接着固定した場合、該テー
プが基礎面および/または貼り付け物品の歪、反
りなどに抗しきれず、経日により貼り付け物品の
端部が基礎面から剥がれてくるといつた欠点があ
る。これは接着剤層に連続して各種の応力が負荷
されると接着剤層内部で流動が起るためであり、
またかかる流動現象は加熱および/または加湿状
態に曝されるような条件下では一層促進されるも
のである。
一方、化学的に架橋反応を誘起せしめる熱硬化
型接着テープは知られているが、該テープは十分
な接着強度を得るために100℃以上の加熱を要し
且つ加熱手段として高価な加熱装置を必要とし、
作業も煩雑となり、しかも基礎面は耐熱性がなけ
れば適用できないという制約がある。
この発明は、基礎面に貼り付け物品を貼り付け
るに際し、熱硬化型接着テープの如き多量の熱容
量を必要とする加熱手段を用いることなく、約40
〜90℃の比較的低温で加熱することにより、表面
状態が粗面である基礎面および/または貼り付け
物品面であつても十分なぬれ性を発揮する粘度に
熱感応して活性化が可能であり、しかも十分な接
着強度を維持し得る熱時感圧性接着材料を用いて
なる貼り付け方法を提供するものである。
この発明の詳細をさらに具体的に説明すると、
基礎面に、常態で良好な感圧接着性を有する感圧
性接着組成物100重量部に対し該組成物との相溶
性が良好であつて且つ融点が70℃以上である反応
型熱溶融性樹脂を50〜200重量部添加してなる常
温で低度の粘着性を有し且つ加熱により感圧接着
性の機能が付与される熱時感圧性接着材料を介し
て貼り付け物品を重ね合わせ、然る後加熱または
加熱加圧することを特徴とする貼り付け方法を提
供するものである。
ここに用いられる感圧性接着組成物は、熱時感
圧性接着材料に所望の粘着性、接着性などを付与
する常態で良好な感圧接着性を有する成分であ
り、例えばアクリル酸ブチル、アクリル酸メチ
ル、アクリル酸エチル、アクリル酸2−エチルヘ
キシル、アクリル酸オクタデシルが最適である
が、他のアクリル酸アルキルエステルでアルキル
基の炭素数が1〜10個のものを使用してもよい
し、併用することも可能である。しかして該アク
リル酸アルキルエステルには、メタクリル酸メチ
ル、メタクリル酸エチル、メタクリル酸ブチルの
如きメタクリル酸アルキルエステル、および(メ
タ)アクリル酸アルキルエステルに共重合可能な
ビニル系モノマー例えばスチレン、酢酸ビニル、
アクリロニトリル、メタクリロニトリルを適量添
加してもよい。
また上記アクリル酸アルキルエステルと共に用
いられる官能基を持つ重合性単量体は、熱時感圧
性接着材料に所望の接着性、凝集性などを付与す
る成分であり、例えば次の重合性単量体が用いら
れる。
(イ) カルボキシル基を持つ重合性単量体、例とし
てアクリル酸、メタクリル酸、クロトン酸、マ
レイン酸、イタコン酸。
(ロ) ヒドロキシル基を持つ重合性単量体、例とし
てアクリル酸−2−ヒドロキシエチルエステ
ル、アクリル酸−2−ヒドロキシプロピルエス
テル、メタクリル酸−2−ヒドロキシエチルエ
ステル、メタクリル酸−2−ヒドロキシプロピ
ルエステル。
(ハ) アミド基を持つ重合性単量体、例としてアク
リル酸アミド、メタクリル酸アミド。
そして前記アクリル酸アルキルエステルと官能
基を持つ重合性単量体とを共重合することによつ
て、この発明に用いられる熱時感圧性接着材料の
母体としてのアクリル系感圧性接着組成物が得ら
れる。しかして感圧性接着組成物としては上記の
アクリル系以外に例えばポリビニルエーテル系、
酢酸ビニル系またはゴム系の常態で良好な感圧接
着性を有する感圧性接着組成物も有効である。
熱溶融性樹脂は、この発明に用いられる熱時感
圧性接着材料に所望の接着保持性を付与する成分
であり、前記組成物との相溶性が良好であつて且
つ融点70℃以上、より好ましくは80〜150℃の樹
脂が使用される。
かかる樹脂としては、上記特性を満足するもの
であれば特に限定されないが、例えば前記重合性
単量体の官能基と直接あるいは架橋剤、触媒の如
き成分を介して反応し得る官能基を少なくとも1
個有するエポキシ樹脂の如き反応型、あるいは前
記重合性単量体の持つ官能基と架橋剤または触媒
を介して反応し得る官能基を少なくとも1個有す
るキシレン樹脂、フエノール樹脂、フエノール変
性樹脂の如き反応型の樹脂を、この発明に用いら
れる熱時感圧性接着材料を構成する熱溶融性樹脂
として用いると、この発明にて貼り付け物品が断
続的あるいは連続的な加熱状態で使用される接着
に適するものである。なお非反応型熱溶融性樹脂
と反応型熱溶融性樹脂とを併用してよいことは勿
論である。
また重合性単量体の持つ官能基と反応型熱溶融
性樹脂との反応を、40〜90℃の比較的低温度下で
促進させるために用いられる前記の架橋剤または
触媒は、感圧性接着組成物100重量部に対し、0.1
〜20重量部添加するのが好ましい。低温下で反応
を促進させるために用いられる該架橋剤として
は、ポリイソシアネート、ポリアミン、メラミン
などが、触媒として金属塩、無機塩、有機塩、第
3級アミン、クレゾールなどの反応触媒が好適に
用いられる。
これらの架橋剤または触媒は、熱時感圧性接着
材料の加熱時に官能基と反応して、接着材料の接
着性特に耐熱性を向上せしめる作用をする。
これらの熱溶融性樹脂は、前記組成物100重量
部に対し、50〜200重量部、より好ましくは70〜
150重量部の範囲で添加することが好ましい。樹
脂が50重量部以下では熱時感圧性接着材料の加熱
時の弾性率が小さく、溶融された該接着材料が固
化する速度が遅く、しかも剪断接着力が弱く、ま
た200重量部以上では接着材料の弾性率が大き
く、溶融された該接着材料の基礎面および/また
は貼り付け物品面へのぬれ性が劣り、剥離強度が
弱くなるために好ましくないものである。
このように構成された熱時感圧性接着材料は、
基礎面および/または貼り付け物品の少なくとも
一方の面に塗設するか、あるいは予め前記接着材
料を低接着性の機能を具備した樹脂加工紙、プラ
スチツクフイルムなどからなる剥離性基材面に塗
布してフイルム状にした接着材料を基礎面と貼り
付け物品間に介在して、約40〜90℃の比較的低い
温度で加熱または加熱加圧(加圧条件:50〜1000
g/cm2)され、この発明の貼り付け方法が完成さ
れる。
前記接着材料のその材料層中にポリエステル、
ナイロン、レーヨンの如き材質からなる0.5〜10
mmの短繊維、またはナイロン不織布、レーヨン不
織布の如き不織布類、寒冷紗、綿布の如き布類、
プラスチツクフイルムなどの補強芯材を入れる
と、接着材料の引張り強度が高められると共に緩
衝効果が得られるので好ましいものである。
この発明の貼り付け方法は、前述の如く装置、
機器などの基礎面に銘板、表示板などの貼り付け
物品を貼り付ける場合に顕著な効果を発揮するも
のであるが、例えば自動車ボデイへのプラスチツ
クサイドモールドなどの貼り付けにも有用であ
る。
以下この発明の実施例を示す。
実施例
アクリル酸エチル:アクリル酸ブチル:グリシ
ジルメタクリレート=3:6.9:0.1(共重合重量
比)の割合で溶液重合(トルエン25%)した感圧
性接着組成物(平均分子量約15万)溶液を用意す
る。
該溶液の固形分100重量部に対して、ビスフエ
ノール型エポキシ樹脂(融点100℃)100重量部、
トリレンジイソシアネート3重量を添加して混合
し、該混合物を厚さ0.2mmのアルミ板(#280サン
ドブラスト)に乾燥後の厚みが50μとなるように
塗布し、、70℃で5分間乾燥して、サンプル片を
作製した。
次にこのサンプル片の熱時感圧性接着材料層面
に、第1表に示す各温度に加熱した厚さ0.2mmの
アルミ板(#280サンドブラスト)を重ね合わ
せ、100g/cm2の圧を加え、室温に戻してシヨツパ
ー型引張試験機(剥離速度50mm/min、20℃×65
%R.H.)にて接着力を測定する。その特性は第
1表に示している。
This invention is a novel method for attaching articles such as nameplates and small articles to the surfaces of articles such as electrical devices, mechanical devices, and housing equipment, or of structures such as concrete surfaces and walls (hereinafter referred to as foundation surfaces). Regarding the attachment method. This invention has a base surface that normally has weak adhesiveness to the extent that an article can be temporarily attached to the base surface, and is heat sensitive by being heated for a short time at a relatively low temperature of about 90°C or less. The bonded articles are laminated through a specific heat-sensitive adhesive material that is activated to a viscosity with a modulus of elasticity equivalent to that of commonly known pressure-sensitive adhesives at room temperature and exhibits sufficient adhesive strength. The object of the present invention is to provide a pasting method that maintains a strong adhesive state even when used at room temperature or under heated conditions by heating or heating and pressurizing the adhesive. Conventionally, when attaching articles such as surface plates such as nameplates, punching plates, and decorative plates, or small articles such as attachment suspension devices and panels to a base surface, a pressure-sensitive adhesive is formed on the support surface. A so-called double-sided pressure-sensitive adhesive tape is used. However, when a tape made of this adhesive is used to adhesively fix an article to be attached to a base surface, the tape may not be able to withstand distortion or warping of the base surface and/or the article to be attached, and may deteriorate over time. There is a drawback that the ends of the applied article may peel off from the base surface. This is because when various stresses are continuously applied to the adhesive layer, flow occurs inside the adhesive layer.
Moreover, such flow phenomenon is further promoted under conditions such as exposure to heating and/or humid conditions. On the other hand, thermosetting adhesive tapes that chemically induce a crosslinking reaction are known, but these tapes require heating to 100°C or higher to obtain sufficient adhesive strength and require expensive heating equipment as a heating means. need,
The work is complicated, and there is a restriction that it cannot be applied unless the base surface is heat resistant. This invention enables the application of an adhesive article to a base surface without using a heating means that requires a large amount of heat capacity, such as a thermosetting adhesive tape.
By heating at a relatively low temperature of ~90°C, it can be thermally activated to a viscosity that exhibits sufficient wettability even on the rough base surface and/or the surface of the attached article. The object of the present invention is to provide a pasting method using a heat-sensitive adhesive material that can maintain sufficient adhesive strength. To explain the details of this invention more specifically,
A reactive hot-melt resin having good compatibility with 100 parts by weight of a pressure-sensitive adhesive composition having good pressure-sensitive adhesive properties under normal conditions and having a melting point of 70°C or higher on the base surface. The pasted articles are laminated via a hot pressure-sensitive adhesive material which has a low degree of tackiness at room temperature and which is given a pressure-sensitive adhesive function by heating, which is made by adding 50 to 200 parts by weight of The present invention provides a pasting method characterized by heating or heating and pressurizing the adhesive after applying the adhesive. The pressure-sensitive adhesive composition used here is a component that has good pressure-sensitive adhesive properties under normal conditions and imparts desired tackiness, adhesion, etc. to the pressure-sensitive adhesive material when hot, such as butyl acrylate, acrylic acid, etc. Methyl, ethyl acrylate, 2-ethylhexyl acrylate, and octadecyl acrylate are most suitable, but other acrylic acid alkyl esters with an alkyl group of 1 to 10 carbon atoms may be used or used in combination. It is also possible. The acrylic acid alkyl esters include methacrylic acid alkyl esters such as methyl methacrylate, ethyl methacrylate, and butyl methacrylate, and vinyl monomers copolymerizable with the (meth)acrylic acid alkyl esters, such as styrene, vinyl acetate, etc.
An appropriate amount of acrylonitrile or methacrylonitrile may be added. In addition, the polymerizable monomer having a functional group used together with the above-mentioned acrylic acid alkyl ester is a component that imparts desired adhesiveness, cohesiveness, etc. to the heat-sensitive adhesive material. For example, the following polymerizable monomer is used. (a) Polymerizable monomers with carboxyl groups, such as acrylic acid, methacrylic acid, crotonic acid, maleic acid, and itaconic acid. (b) Polymerizable monomers having hydroxyl groups, such as 2-hydroxyethyl acrylate, 2-hydroxypropyl acrylate, 2-hydroxyethyl methacrylate, and 2-hydroxypropyl methacrylate. . (c) Polymerizable monomers having an amide group, such as acrylamide and methacrylic acid amide. Then, by copolymerizing the acrylic acid alkyl ester and a polymerizable monomer having a functional group, an acrylic pressure-sensitive adhesive composition as a base material for the hot pressure-sensitive adhesive material used in the present invention is obtained. It will be done. However, in addition to the above-mentioned acrylic adhesive compositions, for example, polyvinyl ether adhesive compositions,
Vinyl acetate-based or rubber-based pressure-sensitive adhesive compositions that have good pressure-sensitive adhesive properties under normal conditions are also effective. The hot-melt resin is a component that imparts desired adhesion retention to the hot pressure-sensitive adhesive material used in the present invention, and has good compatibility with the composition and has a melting point of 70°C or higher, more preferably. 80~150℃ resin is used. Such a resin is not particularly limited as long as it satisfies the above characteristics, but for example, it contains at least one functional group that can react with the functional group of the polymerizable monomer directly or through components such as a crosslinking agent and a catalyst.
reaction type such as epoxy resin, or reaction type such as xylene resin, phenol resin, phenol modified resin, which has at least one functional group that can react with the functional group of the polymerizable monomer via a crosslinking agent or catalyst. When the mold resin is used as a heat-melting resin constituting the hot pressure-sensitive adhesive material used in this invention, it is suitable for adhesives in which the article to be pasted is used in an intermittent or continuous heated state in this invention. It is something. It goes without saying that a non-reactive thermofusible resin and a reactive thermofusible resin may be used in combination. In addition, the above-mentioned crosslinking agent or catalyst used to promote the reaction between the functional group of the polymerizable monomer and the reactive hot-melt resin at a relatively low temperature of 40 to 90°C is used for pressure-sensitive adhesives. 0.1 per 100 parts by weight of the composition
It is preferable to add up to 20 parts by weight. The crosslinking agent used to promote the reaction at low temperature is preferably polyisocyanate, polyamine, melamine, etc., and the catalyst is preferably a reaction catalyst such as metal salt, inorganic salt, organic salt, tertiary amine, cresol, etc. used. These crosslinking agents or catalysts react with functional groups when the hot pressure-sensitive adhesive material is heated, and act to improve the adhesive properties, particularly the heat resistance, of the adhesive material. These hot-melt resins are contained in an amount of 50 to 200 parts by weight, more preferably 70 to 200 parts by weight, based on 100 parts by weight of the composition.
It is preferably added in an amount of 150 parts by weight. If the resin is less than 50 parts by weight, the elastic modulus of the pressure-sensitive adhesive material when heated is small, the rate at which the melted adhesive material solidifies is slow, and the shear adhesive strength is weak, and if the resin is more than 200 parts by weight, the adhesive material This is undesirable because the elastic modulus of the adhesive material is large, the wettability of the melted adhesive material to the base surface and/or the surface of the article to be adhered to is poor, and the peel strength is weakened. The heat-sensitive adhesive material configured in this way is
Either the adhesive material is applied to at least one of the base surface and/or the surface of the article to be pasted, or the adhesive material is applied in advance to the surface of a removable base material such as resin-treated paper or plastic film that has a low adhesive function. A film-like adhesive material is interposed between the base surface and the article to be pasted, and heated or heated and pressurized at a relatively low temperature of about 40 to 90 degrees Celsius (pressure conditions: 50 to 1000 degrees Celsius).
g/cm 2 ), and the pasting method of the present invention is completed. polyester in that material layer of said adhesive material;
0.5~10 made of materials such as nylon and rayon
mm short fibers, or non-woven fabrics such as nylon non-woven fabrics and rayon non-woven fabrics, fabrics such as cheesecloth and cotton fabrics,
It is preferable to include a reinforcing core material such as a plastic film, since this increases the tensile strength of the adhesive material and provides a cushioning effect. The pasting method of the present invention includes the above-mentioned device,
It exhibits a remarkable effect when attaching items such as name plates and display boards to the basic surface of equipment, etc., but it is also useful for attaching plastic side molds to automobile bodies, for example. Examples of this invention will be shown below. Example: Prepare a solution of a pressure-sensitive adhesive composition (average molecular weight approximately 150,000) solution polymerized (toluene 25%) at a ratio of ethyl acrylate: butyl acrylate: glycidyl methacrylate = 3:6.9:0.1 (copolymerization weight ratio). do. For 100 parts by weight of solid content of the solution, 100 parts by weight of bisphenol type epoxy resin (melting point 100°C),
Add and mix 3 weights of tolylene diisocyanate, apply the mixture to a 0.2 mm thick aluminum plate (#280 sandblast) so that the thickness after drying is 50μ, and dry at 70℃ for 5 minutes. , a sample piece was prepared. Next, a 0.2 mm thick aluminum plate (#280 sandblast) heated to each temperature shown in Table 1 was placed on the surface of the hot pressure sensitive adhesive material layer of this sample piece, and a pressure of 100 g/cm 2 was applied. Return to room temperature and test using a shotpar type tensile tester (peel speed 50mm/min, 20℃ x 65cm)
%RH). Its properties are shown in Table 1.
【表】
一方前記混合物を低接着性を具備した樹脂加工
紙上に乾燥後の厚みが50μとなるように塗布し、
70℃で5分間乾燥して、フイルム状の熱時感圧性
接着材料を製造する。
このフイルム状接着材料を厚さ0.7mmのアルミ
板(#280サンドブラスト)に仮着させ、これを
曲率半径が100mm、50mmおよび30mmにそれぞれ賦
形されたABS樹脂シート(厚さ0.13mm)および、
アルミ板(厚さ0.7mm、#280サンドブラスト)か
らなる試験用の基礎面に100℃で60秒間(100g/
cm2で加圧)加熱圧着して試料片を作成した。
この試料片を下記サイクルを1サイクルとする
温度サイクル試験を10サイクル行ない端部剥れの
状態を観察した。その特性を第2表に示してい
る。[Table] On the other hand, the mixture was applied onto a resin-treated paper with low adhesion so that the thickness after drying was 50μ,
Dry at 70°C for 5 minutes to produce a film-like heat-sensitive adhesive material. This film-like adhesive material was temporarily attached to a 0.7 mm thick aluminum plate (#280 sandblast), which was then shaped into an ABS resin sheet (0.13 mm thick) with a radius of curvature of 100 mm, 50 mm, and 30 mm, respectively.
A test base consisting of an aluminum plate (0.7 mm thick, #280 sandblasted) was heated at 100℃ for 60 seconds (100g/
A sample piece was created by heat-pressing (pressure at cm2 ). This sample piece was subjected to a temperature cycle test for 10 cycles, with the following cycle being one cycle, and the state of peeling at the edges was observed. Its properties are shown in Table 2.
【表】
判定方法
◎:端部剥れなし。
○:端部が僅かに上つている。
上記実施例からも明らかなように、この発明の
貼り付け方法によれば苛酷な温度サイクル試験に
ても良好に接着している事実が明らかである。[Table] Judgment method ◎: No peeling at edges.
○: The edges are slightly raised.
As is clear from the above examples, it is clear that the bonding method of the present invention provides good adhesion even in severe temperature cycle tests.
Claims (1)
感圧性接着組成物100重量部に対し、該組成物と
の相溶性が良好であつて且つ融点が70℃以上であ
る反応型熱溶融性樹脂を50〜200重量部添加して
なる常温で低度の粘着性を有し且つ加熱により感
圧接着性の機能が付与される熱時感圧性接着材料
を介して貼り付け物品を重ね合わせ、然る後加熱
または加熱加圧することを特徴とする貼り付け方
法。 2 熱時感圧性接着材料がその材料層中に短繊維
または補強芯材を有している特許請求の範囲第1
項記載の貼り付け方法。[Scope of Claims] 1. Good compatibility with 100 parts by weight of a pressure-sensitive adhesive composition that has good pressure-sensitive adhesive properties under normal conditions on the base surface and has a melting point of 70°C or higher. Through a hot pressure-sensitive adhesive material which has a low degree of tackiness at room temperature and which is given pressure-sensitive adhesive function by heating, it is made by adding 50 to 200 parts by weight of a reactive heat-melt resin. A pasting method characterized by overlapping articles to be pasted and then heating or heating and pressurizing them. 2. Claim 1, in which the heat-sensitive adhesive material has short fibers or a reinforcing core material in its material layer.
Pasting method described in section.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP5738777A JPS53142445A (en) | 1977-05-17 | 1977-05-17 | Bonding method |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP5738777A JPS53142445A (en) | 1977-05-17 | 1977-05-17 | Bonding method |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS53142445A JPS53142445A (en) | 1978-12-12 |
| JPS6158506B2 true JPS6158506B2 (en) | 1986-12-11 |
Family
ID=13054191
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP5738777A Granted JPS53142445A (en) | 1977-05-17 | 1977-05-17 | Bonding method |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS53142445A (en) |
Families Citing this family (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP4729266B2 (en) * | 2004-05-11 | 2011-07-20 | ニッタ株式会社 | Thermally conductive composition and thermal conductive sheet |
| JP4837516B2 (en) * | 2006-10-12 | 2011-12-14 | マクセルスリオンテック株式会社 | Non-stretchable supportless adhesive tape and method for producing the same |
Family Cites Families (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5314417B2 (en) * | 1973-07-14 | 1978-05-17 | ||
| JPS5117225A (en) * | 1974-08-01 | 1976-02-12 | Mitsui Petrochemical Ind | SETSUCHAKUZAI |
| JPS5153591A (en) * | 1974-11-05 | 1976-05-12 | Mitsui Petrochemical Ind | Tankasuisojushino seizohoho |
-
1977
- 1977-05-17 JP JP5738777A patent/JPS53142445A/en active Granted
Also Published As
| Publication number | Publication date |
|---|---|
| JPS53142445A (en) | 1978-12-12 |
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