JPH0222096B2 - - Google Patents
Info
- Publication number
- JPH0222096B2 JPH0222096B2 JP56167473A JP16747381A JPH0222096B2 JP H0222096 B2 JPH0222096 B2 JP H0222096B2 JP 56167473 A JP56167473 A JP 56167473A JP 16747381 A JP16747381 A JP 16747381A JP H0222096 B2 JPH0222096 B2 JP H0222096B2
- Authority
- JP
- Japan
- Prior art keywords
- resin
- thermoplastic polyester
- thick
- weight
- polyester resin
- 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
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C45/00—Injection moulding, i.e. forcing the required volume of moulding material through a nozzle into a closed mould; Apparatus therefor
- B29C45/0001—Injection moulding, i.e. forcing the required volume of moulding material through a nozzle into a closed mould; Apparatus therefor characterised by the choice of material
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C45/00—Injection moulding, i.e. forcing the required volume of moulding material through a nozzle into a closed mould; Apparatus therefor
- B29C45/16—Making multilayered or multicoloured articles
- B29C2045/1698—Making multilayered or multicoloured articles multicoloured articles moulded in one step
Landscapes
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Mechanical Engineering (AREA)
- Manufacture Of Macromolecular Shaped Articles (AREA)
- Injection Moulding Of Plastics Or The Like (AREA)
Description
【発明の詳細な説明】
本発明は、大理石模様を有する厚肉成形体の製
造方法であつて、茲に厚肉成形体とは、例えば、
野外用フラワーポツト又はガーデンセツト用のテ
ーブル、椅子等の成形体である。DETAILED DESCRIPTION OF THE INVENTION The present invention is a method for producing a thick-walled molded article having a marble pattern, and the thick-walled molded article is, for example,
Molded objects such as tables and chairs for outdoor flower pots or garden sets.
従来エチレンテレフタレートを主たる繰り返し
単位とする固有粘度0.55以上の熱可塑性ポリエス
テル樹脂を樹脂成分として含有する成形用組成物
は、前記の如き厚肉成形体を得ることが困難とさ
れているが、本発明は該厚肉成形体組成物から大
理石模様を有する合成樹脂製厚肉成形体を容易に
得る方法を提供するものである。 Conventionally, it has been difficult to obtain a thick-walled molded article with a molding composition containing a thermoplastic polyester resin having an intrinsic viscosity of 0.55 or more and having ethylene terephthalate as a main repeating unit as a resin component. The present invention provides a method for easily obtaining a thick-walled synthetic resin molded article having a marble pattern from the thick-walled molded article composition.
エチレンテレフタレートを主たる繰り返し単位
とする固有粘度0.55以上の熱可塑性ポリエステル
樹脂(以下単に熱可塑性ポリエステル樹脂とい
う)は、その成形体が透明性、機械的強度、ガス
バリヤー性、無毒性等に優れていること、及び廃
棄焼却される際の燃焼カロリーが低いこと等の特
質により、飲料品や化粧料用等の比較的薄肉の各
種容器として広範囲に利用されているが、熱可塑
性ポリエステル樹脂による厚肉成形体の成形が困
難であることから、使用済みの熱可塑性ポリエス
テル樹脂成形体は、他の合成樹脂成形体の材料と
して再利用されることなく、直ちに焼却による廃
棄処理に付されているのが現状である。 Thermoplastic polyester resin whose main repeating unit is ethylene terephthalate and has an intrinsic viscosity of 0.55 or more (hereinafter simply referred to as thermoplastic polyester resin) has excellent transparency, mechanical strength, gas barrier properties, non-toxicity, etc. Due to its characteristics such as low calorie burn when disposed of and incinerated, it is widely used as a variety of relatively thin-walled containers for beverages and cosmetics, etc. However, thick-walled containers made of thermoplastic polyester resin Due to the difficulty of molding plastic bodies, used thermoplastic polyester resin moldings are currently disposed of immediately by incineration rather than being reused as materials for other synthetic resin moldings. It is.
本発明は特許請求の範囲に記載した構成とする
ことにより、従来厚肉成形体の成形が困難である
とされていた熱可塑性ポリエステル樹脂を合成樹
脂主成分として含む成形用組成物を利用し、例え
ば野外用フラワーポツト、ガーデンセツト用テー
ブルや椅子等を容易に得ることの出来る製造方法
を提供するもので、特に成形用組成物中の合成樹
脂成分として使用済みの熱可塑性ポリエステル樹
脂成形体、ポリエチレン樹脂成形体、ポリプロピ
レン樹脂成形体を破砕して得られる合成樹脂成形
体破砕物や、各合成樹脂成形体の成形段階で出る
合成樹脂屑等をも利用し得る点に特徴を有するも
のである。 By having the structure described in the claims, the present invention utilizes a molding composition containing a thermoplastic polyester resin as a main synthetic resin component, which was conventionally considered difficult to mold into thick-walled molded objects, For example, it provides a manufacturing method that can easily produce outdoor flower pots, tables and chairs for garden sets, etc. In particular, used thermoplastic polyester resin moldings and polyethylene as synthetic resin components in molding compositions are provided. This method is characterized in that it can also utilize crushed synthetic resin moldings obtained by crushing resin moldings and polypropylene resin moldings, as well as synthetic resin waste generated during the molding step of each synthetic resin molding.
本発明のパール感のある大理石模様を有する合
成樹脂製厚肉成形体の製造方法においては、組成
物中の合成樹脂成分が、含水率0.04〜0.4重量%
に調整されている固有粘度0.55以上の熱可塑性ポ
リエステル樹脂20〜70重量%と、ポリエチレン樹
脂15重量%以上と、ポリプロピレン樹脂15重量%
以上との混合樹脂によつて構成されている成形用
組成物を利用するもので、例えば前記特定割合の
混合樹脂に、更に必要により着色剤やその他の添
加剤が適宜添加、混合されている成形用組成物を
利用するものである。本発明において使用する成
形用組成物中の合成樹脂主成分たる熱可塑性ポリ
エステル樹脂は、組成物中の全樹脂成分の20〜70
重量%の範囲内に調整され、しかもその含水率が
0.01〜0.4重量%の範囲内に調整されていること
が必要である。これは、本発明の厚肉成形体の製
造方法においては、使用する成形用組成物中の熱
可塑性ポリエステル樹脂に或る程度の水分を含有
せしめておき、厚肉成形体の成形工程たる溶融、
混練り、賦形工程中に熱可塑性ポリエステル樹脂
におけるエステル結合の一部に加水分解を生じさ
せ、これを、オリゴマーを含んだ熱可塑性ポリエ
ステル樹脂となし、加水分解によつて新たに生成
したオリゴマーに、厚肉成形体中におけるフイラ
ーの作用を奏せしめると同時に、本発明の成形用
組成物に賦形性を付与せしめるものである。 In the method for producing a thick-walled synthetic resin molded article having a pearly marble pattern according to the present invention, the synthetic resin component in the composition has a water content of 0.04 to 0.4% by weight.
20 to 70% by weight of thermoplastic polyester resin with an intrinsic viscosity of 0.55 or more, 15% by weight or more of polyethylene resin, and 15% by weight of polypropylene resin.
A molding composition that uses a molding composition composed of a mixed resin with the above, for example, a molding composition in which a coloring agent and other additives are added and mixed as necessary to the mixed resin in the specified proportion. It utilizes a composition for use. The thermoplastic polyester resin, which is the main synthetic resin component in the molding composition used in the present invention, accounts for 20 to 70% of the total resin components in the composition.
The water content is adjusted within the range of weight %, and the moisture content is
It is necessary to adjust the content within the range of 0.01 to 0.4% by weight. This is because, in the method for producing a thick-walled molded body of the present invention, the thermoplastic polyester resin in the molding composition used is made to contain a certain amount of water, and the melting and molding steps of the thick-walled molded body are performed.
During the kneading and shaping process, some of the ester bonds in the thermoplastic polyester resin are hydrolyzed, and this is converted into a thermoplastic polyester resin containing oligomers. , which exhibits the function of a filler in a thick-walled molded article, and at the same time imparts shapeability to the molding composition of the present invention.
合成樹脂成分中のポリエチレン樹脂は、合成樹
脂中の主成分たる熱可塑性ポリエステル樹脂との
極端な非混融性のためにパール感のある大理石模
様を現出させる作用を果すポリプロピレン樹脂
と、前記熱可塑性ポリエステル樹脂との間で生ず
る層間剥離を防止するための接着剤の作用を奏
し、且つ得られる厚肉成形体の表面に平滑性を具
備させ、肌理の緻密な成形体たらしめる作用を奏
するものであるから、本発明で利用する成形用組
成物においては、該組成物中の合成樹脂成分が熱
可塑性ポリエステル樹脂とポリエチレン樹脂とポ
リプロピレン樹脂との3者の混合樹脂で構成され
ていることが必要である。 The polyethylene resin in the synthetic resin component is extremely immiscible with the thermoplastic polyester resin, which is the main component in the synthetic resin, and the polypropylene resin has the effect of creating a pearly marble pattern. A substance that acts as an adhesive to prevent delamination between the plastic polyester resin and the plastic polyester resin, and also provides smoothness to the surface of the resulting thick-walled molded product, making it a densely textured molded product. Therefore, in the molding composition used in the present invention, it is necessary that the synthetic resin component in the composition is composed of a mixed resin of three components: a thermoplastic polyester resin, a polyethylene resin, and a polypropylene resin. It is.
本発明で使用する成形用組成物中の合成樹脂成
分たる熱可塑性ポリエステル樹脂とポリエチレン
樹脂とポリプロピレン樹脂との混合樹脂におい
て、熱可塑性ポリエステル樹脂が70重量%を越え
ると、成形用組成物は硬くなり、粘りの無いもの
となつてしまい、得られる成形体が脆く、亀裂の
発生し易い、強度の無い劣悪品になるという欠点
を生ずるし、また、20重量%未満では組成物自体
の流動性が悪く、目的製品たる厚肉成形体の成形
操作が困難になるという欠点が生ずる。また、使
用される熱可塑性ポリエステル樹脂は、その含水
率が0.04重量%未満のものになると、成形用組成
物の溶融、混練り、成形工程中で、熱可塑性ポリ
エステル樹脂の加水分解が困難となり、目的製品
たる厚肉成形体の成形操作が難しくなるし、また
該含水率が0.4重量%を越えると、成形工程中に
おける発泡現象が激しく、得られる厚肉成形体の
表面がごつごつした肌理の荒いものとなるばかり
でなく、成形体の成形操作自体が困難になるとい
う欠点を生ずる。また、本発明で使用する成形用
組成物中で、得られる厚肉成形体に、該組成物中
の主合成樹脂成分たる熱可塑性ポリエステル樹脂
と相俟つてパール感のある大理石模様を現出させ
るポリプロピレン樹脂については、これが全樹脂
成分中の15重量%未満になると得られる厚肉成形
体に具現されるパール感のある大理石模様の現用
が乏しく、また、熱可塑性ポリエステル樹脂とポ
リプロピレン樹脂との間の接着作用を奏するポリ
エチレン樹脂については、これが全樹脂成分中の
15重量%未満では、該樹脂による前記接着作用が
十分でなく、得られる厚肉成形体において、熱可
塑性ポリエステル樹脂成分とポリプロピレン樹脂
成分との間で層間剥離現象が発生しやすくなると
いう欠点を生ずる。 In the mixed resin of thermoplastic polyester resin, polyethylene resin, and polypropylene resin that is the synthetic resin component in the molding composition used in the present invention, if the thermoplastic polyester resin exceeds 70% by weight, the molding composition becomes hard. If it is less than 20% by weight, the composition itself will have poor fluidity, resulting in a poor product that is brittle, prone to cracking, and has no strength. Unfortunately, there arises a drawback that the molding operation of the desired product, the thick-walled molded body, becomes difficult. Additionally, if the moisture content of the thermoplastic polyester resin used is less than 0.04% by weight, it will be difficult to hydrolyze the thermoplastic polyester resin during the melting, kneading, and molding processes of the molding composition. The molding operation of the target product, a thick-walled molded product, becomes difficult, and if the water content exceeds 0.4% by weight, foaming phenomenon during the molding process will be severe, and the surface of the resulting thick-walled molded product will have a rough and rough texture. This results in the drawback that not only does it become difficult to use, but also that the operation of molding the molded object itself becomes difficult. In addition, in the molding composition used in the present invention, the resulting thick-walled molded product exhibits a pearly marble pattern in combination with the thermoplastic polyester resin that is the main synthetic resin component in the composition. Regarding polypropylene resin, if it is less than 15% by weight of the total resin component, the pearly marble pattern that is produced in thick-walled molded products is rarely used, and the difference between thermoplastic polyester resin and polypropylene resin Regarding polyethylene resin, which has an adhesive effect, this
If it is less than 15% by weight, the adhesion effect of the resin will not be sufficient, resulting in the drawback that delamination phenomenon will easily occur between the thermoplastic polyester resin component and the polypropylene resin component in the resulting thick-walled molded product. .
本発明の合成樹脂製厚肉成形体の製造方法は、
前記、特別に含水率が調整されている熱可塑性ポ
リエステル樹脂と、ポリエチレン樹脂と、ポリプ
ロピレン樹脂との混合樹脂を合成樹脂成分とする
成形用組成物、即ち前記混合樹脂からなる合成樹
脂成分に、必要に応じて染、顔料やその他の添加
剤を適宜添加、含有せしめた成形用組成物を、熱
可塑性ポリエステル樹脂の融点よりは低く、且つ
ポリエチレン樹脂やポリプロピレン樹脂の融点よ
りは高い温度にあたる約250〜290℃で射出成形、
具体的には15Kg/cm2程度の圧力を利用した射出成
形を行い、次いで徐冷することから成るもので、
熱可塑性ポリエステル樹脂とポリプロピレン樹脂
との間の極端な非混融性に基いて現出されている
パール感のある大理石模様を具備する厚肉成形体
を得るものである。 The method for producing a thick-walled synthetic resin molded article of the present invention includes:
The molding composition whose synthetic resin component is a mixed resin of a thermoplastic polyester resin, a polyethylene resin, and a polypropylene resin whose moisture content has been specially adjusted, that is, a synthetic resin component consisting of the mixed resin, is necessary. A molding composition containing appropriate dyes, pigments, and other additives is heated to a temperature of about 250 to 250°C, which is lower than the melting point of thermoplastic polyester resin and higher than the melting point of polyethylene resin or polypropylene resin. Injection molding at 290℃,
Specifically, it consists of injection molding using a pressure of about 15 kg/cm 2 , followed by slow cooling.
A thick-walled molded article having a marble pattern with a pearly feel, which is created based on the extreme non-fusibility between the thermoplastic polyester resin and the polypropylene resin, is obtained.
本発明の合成樹脂製厚肉成形体の製造方法は叙
上の通りの構成から成るもので、成形用組成物中
の合成樹脂成分として、所定の含水率に調整され
ている熱可塑性ポリエステル樹脂を主成分とし、
これにポリエチレン樹脂とポリプロピレン樹脂と
が混合されている混合樹脂、即ち、従来、厚肉成
形体の成形が困難であるとされていた熱可塑性ポ
リエステル樹脂を合成樹脂主成分として含有する
成形用組成物を使用し、これを射出成形すること
により、パール感を有する大理石模様が現出され
ている厚肉成形体を製造するものであるから、従
来、その用途が皆無であるとされていた使用済み
の熱可塑性ポリエステル樹脂成形体の破砕物を熱
可塑性ポリエステル樹脂成分として使用すること
が出来るので、材料費にかかる経費を廉価に抑え
られるばかりでなく、使用済みの熱可塑性ポリエ
ステル成形体の再利用を計れるという点で公害防
止のうえからも多大の作用、効果を有するもので
ある。 The method for producing a thick-walled synthetic resin molded article according to the present invention has the above-mentioned configuration, in which a thermoplastic polyester resin adjusted to a predetermined moisture content is used as the synthetic resin component in the molding composition. The main ingredient is
A molding composition containing a thermoplastic polyester resin as the main synthetic resin component, which is a mixture of polyethylene resin and polypropylene resin, that is, a thermoplastic polyester resin that has been considered difficult to mold into thick-walled molded objects. By injection molding this product, a thick-walled molded product with a pearly marble pattern is produced. Since the crushed products of thermoplastic polyester molded bodies can be used as the thermoplastic polyester resin component, not only can material costs be kept low, but it is also possible to reuse used thermoplastic polyester molded bodies. Since it can be measured, it has a great effect in terms of pollution prevention.
以下、本発明の合成樹脂製厚肉成形体の製造方
法の具体的な構成を実施例に基いて説明する。 Hereinafter, the specific structure of the method for producing a thick-walled synthetic resin molded article of the present invention will be explained based on Examples.
実施例
熱可塑性ポリエステル樹脂製の透明な使用済み
の1醤油瓶105本を洗浄し、これを直ちに破砕
処理に付し、表面に付着水を有する1辺5mm前後
の細片からなる熱可塑性ポリエステル樹脂の破砕
物となし、次いで60分間の大気乾燥処理を施し
て、含水率0.2重量%の熱可塑性ポリエステル樹
脂破砕物4208gを得た。Example 105 used transparent soy sauce bottles made of thermoplastic polyester resin were washed and immediately subjected to crushing treatment to produce thermoplastic polyester resin consisting of small pieces of about 5 mm on each side with water attached to the surface. This was followed by drying in the air for 60 minutes to obtain 4208 g of a crushed thermoplastic polyester resin having a water content of 0.2% by weight.
一方、同じく使用済みのポリエチレン樹脂製の
180c.c.−化粧料用瓶47本を洗浄後、破砕処理し、
表面に付着水を有する1辺5mm前後の細片からな
るポリエチレン樹脂の破砕物となし、次いで60分
間の大気乾燥処理を施して、ポリエチレン樹脂破
砕物1410gを得た。 On the other hand, it is also made of used polyethylene resin.
180 c.c. - 47 cosmetic bottles were cleaned and crushed,
A crushed polyethylene resin consisting of pieces of about 5 mm on each side with water attached to the surface was prepared, and then dried in the air for 60 minutes to obtain 1410 g of a crushed polyethylene resin.
さらに、同じく使用済みのポリプロピレン樹脂
製の180c.c.−化粧料用瓶47本を洗浄後、破砕処理
に付し、表面に付着水を有する1辺5mmの前後の
細片からなるポリエチレン樹脂の破砕物とし、次
いで60分間の大気乾燥処理を施してポリエチレン
樹脂破砕物1410gを得た。 Furthermore, 47 used 180 c.c. cosmetic bottles made of polypropylene resin were washed and crushed, and polyethylene resin made of small pieces of 5 mm on each side with water attached to the surface was washed. The resulting product was crushed and then dried in the air for 60 minutes to obtain 1410 g of crushed polyethylene resin.
以上の処理により得られた熱可塑性ポリエステ
ル樹脂破砕物4208gと、ポリエチレン樹脂破砕物
1410gと、ポリプロピレン樹脂破砕物1410gとか
らなる成形用組成物を、約250℃の加熱下に溶融、
混練し、圧力15Kg/cm2の射出成形に付し、徐冷
後、金型から取り外して水冷処理し、厚さ12mm、
口部直径30cm、高さ44cmの樽型の厚肉成形体を成
形した。 4208g of crushed thermoplastic polyester resin obtained by the above treatment and crushed polyethylene resin
A molding composition consisting of 1,410 g of crushed polypropylene resin and 1,410 g of crushed polypropylene resin was melted under heating at approximately 250°C.
The mixture was kneaded and injection molded at a pressure of 15 kg/cm 2 , and after slow cooling, it was removed from the mold and water-cooled to a thickness of 12 mm.
A thick-walled barrel-shaped body with a mouth diameter of 30 cm and a height of 44 cm was molded.
得られた厚肉成形体は、表面が平滑で、全体に
わたつて熱可塑性ポリエステル樹脂とポリエチレ
ン樹脂との間の極端な非混融性に基くパール感を
有する大理石模様が現出されており、同様にして
成形された別製の円盤状の厚肉成形体からなるテ
ーブル板に対して脚体として合致し、両者の組み
合わせ体は陶器等に代わるガーデンセツト用テー
ブル、椅子として、また前記の樽型の一部はガー
デンセツト用の椅子として利用できるものであつ
た。 The obtained thick-walled molded product has a smooth surface, and a marble pattern with a pearly feel based on the extreme non-miscibility between the thermoplastic polyester resin and the polyethylene resin appears over the entire surface. It fits as a leg to a table board made of a separate thick-walled disc-shaped molded body molded in the same way, and the combination of the two can be used as a table or chair for garden sets in place of ceramics, etc., or as a barrel as described above. Some of the molds could be used as chairs for garden sets.
Claims (1)
に当たり、含水率0.04〜0.4重量%に調整されて
いるエチレンテレフタレートを主たる繰り返し単
位とする固有粘度0.55以上の熱可塑性ポリエステ
ル樹脂20〜70重量%と、15重量%以上のポリエチ
レン樹脂と、同じく15重量%以上のポリプロピレ
ン樹脂とからなる混合樹脂を合成樹脂成分とする
成形用組成物を250〜290℃の成形温度で射出成形
し、徐冷することを特徴とする大理石模様を有す
る合成樹脂製厚肉成形体の製造方法。1. For the production of thick-walled synthetic resin molded articles with a thickness of 5 mm or more, 20 to 70 weight thermoplastic polyester resins with an intrinsic viscosity of 0.55 or more, whose main repeating unit is ethylene terephthalate, whose water content is adjusted to 0.04 to 0.4% by weight. A molding composition whose synthetic resin component is a mixed resin consisting of 15% by weight or more of polyethylene resin and 15% by weight or more of polypropylene resin is injection molded at a molding temperature of 250 to 290°C, and then slowly cooled. 1. A method for producing a thick-walled synthetic resin molded article having a marble pattern.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP16747381A JPS5869027A (en) | 1981-10-20 | 1981-10-20 | Manufacture of synthetic resin thick molded body with marble pattern |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP16747381A JPS5869027A (en) | 1981-10-20 | 1981-10-20 | Manufacture of synthetic resin thick molded body with marble pattern |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS5869027A JPS5869027A (en) | 1983-04-25 |
| JPH0222096B2 true JPH0222096B2 (en) | 1990-05-17 |
Family
ID=15850325
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP16747381A Granted JPS5869027A (en) | 1981-10-20 | 1981-10-20 | Manufacture of synthetic resin thick molded body with marble pattern |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS5869027A (en) |
Families Citing this family (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| KR20020089013A (en) * | 2001-05-22 | 2002-11-29 | 이무호 | A Method for Producing a Synthetic Resins with a Marble pattern and A Product thereof |
| CN108422621B (en) * | 2018-03-15 | 2020-05-05 | 浙江万豪模塑股份有限公司 | Three-color mold with stainless steel inserts and three-color triangular window decorative plate |
Family Cites Families (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5432562A (en) * | 1977-08-17 | 1979-03-09 | Teijin Ltd | Thermoplastic resin container having metallic luster |
-
1981
- 1981-10-20 JP JP16747381A patent/JPS5869027A/en active Granted
Also Published As
| Publication number | Publication date |
|---|---|
| JPS5869027A (en) | 1983-04-25 |
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