JPH0331348B2 - - Google Patents
Info
- Publication number
- JPH0331348B2 JPH0331348B2 JP15230085A JP15230085A JPH0331348B2 JP H0331348 B2 JPH0331348 B2 JP H0331348B2 JP 15230085 A JP15230085 A JP 15230085A JP 15230085 A JP15230085 A JP 15230085A JP H0331348 B2 JPH0331348 B2 JP H0331348B2
- Authority
- JP
- Japan
- Prior art keywords
- layer
- ethylene
- polyethylene
- weight
- polypropylene
- 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
- -1 polyethylene Polymers 0.000 claims description 46
- 239000004743 Polypropylene Substances 0.000 claims description 24
- 229920001155 polypropylene Polymers 0.000 claims description 24
- 239000004698 Polyethylene Substances 0.000 claims description 23
- 229920000573 polyethylene Polymers 0.000 claims description 23
- 229920005676 ethylene-propylene block copolymer Polymers 0.000 claims description 18
- 229920000092 linear low density polyethylene Polymers 0.000 claims description 14
- 239000004707 linear low-density polyethylene Substances 0.000 claims description 14
- 238000004519 manufacturing process Methods 0.000 claims description 13
- 239000000203 mixture Substances 0.000 claims description 12
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 claims description 9
- 239000005977 Ethylene Substances 0.000 claims description 9
- 238000001816 cooling Methods 0.000 claims description 3
- 238000010030 laminating Methods 0.000 claims 1
- 239000010410 layer Substances 0.000 description 47
- 239000000853 adhesive Substances 0.000 description 11
- 230000001070 adhesive effect Effects 0.000 description 11
- 239000012790 adhesive layer Substances 0.000 description 7
- 238000000034 method Methods 0.000 description 6
- 239000004711 α-olefin Substances 0.000 description 3
- WSSSPWUEQFSQQG-UHFFFAOYSA-N 4-methyl-1-pentene Chemical compound CC(C)CC=C WSSSPWUEQFSQQG-UHFFFAOYSA-N 0.000 description 2
- 239000000654 additive Substances 0.000 description 2
- 239000003963 antioxidant agent Substances 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 239000005038 ethylene vinyl acetate Substances 0.000 description 2
- 229920005674 ethylene-propylene random copolymer Polymers 0.000 description 2
- 229920001519 homopolymer Polymers 0.000 description 2
- 239000000155 melt Substances 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 229920001200 poly(ethylene-vinyl acetate) Polymers 0.000 description 2
- VXNZUUAINFGPBY-UHFFFAOYSA-N 1-Butene Chemical compound CCC=C VXNZUUAINFGPBY-UHFFFAOYSA-N 0.000 description 1
- KWKAKUADMBZCLK-UHFFFAOYSA-N 1-octene Chemical compound CCCCCCC=C KWKAKUADMBZCLK-UHFFFAOYSA-N 0.000 description 1
- 229920000089 Cyclic olefin copolymer Polymers 0.000 description 1
- XTXRWKRVRITETP-UHFFFAOYSA-N Vinyl acetate Chemical compound CC(=O)OC=C XTXRWKRVRITETP-UHFFFAOYSA-N 0.000 description 1
- 239000002981 blocking agent Substances 0.000 description 1
- IAQRGUVFOMOMEM-UHFFFAOYSA-N butene Natural products CC=CC IAQRGUVFOMOMEM-UHFFFAOYSA-N 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 229920001577 copolymer Polymers 0.000 description 1
- 238000007334 copolymerization reaction Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 235000013305 food Nutrition 0.000 description 1
- 238000010528 free radical solution polymerization reaction Methods 0.000 description 1
- 238000012685 gas phase polymerization Methods 0.000 description 1
- 229920001903 high density polyethylene Polymers 0.000 description 1
- 239000004700 high-density polyethylene Substances 0.000 description 1
- 229920001684 low density polyethylene Polymers 0.000 description 1
- 239000004702 low-density polyethylene Substances 0.000 description 1
- 239000000314 lubricant Substances 0.000 description 1
- 238000000465 moulding Methods 0.000 description 1
- 229920006280 packaging film Polymers 0.000 description 1
- 239000012785 packaging film Substances 0.000 description 1
- YWAKXRMUMFPDSH-UHFFFAOYSA-N pentene Chemical compound CCCC=C YWAKXRMUMFPDSH-UHFFFAOYSA-N 0.000 description 1
- 229920005638 polyethylene monopolymer Polymers 0.000 description 1
- 238000006116 polymerization reaction Methods 0.000 description 1
- 229920000098 polyolefin Polymers 0.000 description 1
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 1
- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 description 1
- 229920001384 propylene homopolymer Polymers 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 239000012748 slip agent Substances 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
Landscapes
- Manufacture Of Macromolecular Shaped Articles (AREA)
- Laminated Bodies (AREA)
Description
〔産業上の利用分野〕
本発明は、ポリエチレンとポリプロピレンとを
接着剤層を介して貼り合わせた積層フイルムの製
造方法に関する。
〔従来の技術およびその問題点〕
ポリエチレンとポリプロピレンとは同じポリオ
レフインではあるが、殆んど相溶性が見られず、
積層フイルムにした場合相互の接着性は極めて劣
るものであり、また、フイルム外観も良好なもの
ではない。そのためにポリエチレンとポリプロピ
レンとの積層フイルムの用途は大幅に制限されて
いた。従来、両フイルムの間に各種の接着剤層を
介在させて接着性を改良することが試みられてき
た。しかし、充分な接着力が得られしかもフイル
ム外観が良好である積層フイルムは未だ開発され
ていない。
〔問題点を解決するための手段〕
本発明は、ポリエチレン層とポリプロピレン層
とが充分強力に接着され、しかも透明性および外
観が良好な積層フイルムの製造方法を提供する。
本発明は、線状低密度ポリエチレン40〜80重量
%とエチレン含有量が3〜10重量%の範囲のエチ
レン−プロピレンブロツク共重合体60〜20重量%
とを配合した組成物(以下接着剤組成物という)
を、溶融状態のポリエチレン層とポリプロピレン
層との間に介在させて積層し、冷却固化すること
を特徴とする積層フイルムの製造方法に関するも
のである。
線状低密度ポリエチレンとしては、遷移金属触
媒を用いて、50モル%以上のエチレンとα−オレ
フインとを溶液重合、気相重合あるいはスラリー
重合など公知の方法で共重合させた、エチレン−
α−オレフイン共重合体を使用し得る。共重合に
使用されるα−オレフインとしては、プロピレ
ン、ブテン、ぺンテン、4−メチルぺンテン−
1、オクテンなどが挙げられる。線状低密度ポリ
エチレンはその優れた透明性、耐熱性、機械的強
度などのため、本発明に用いられる極薄の接着剤
層フイルム用の原料として好適である。線状低密
度ポリエチレンのメルトインデツクスは0.5〜20
g/10分の範囲がフイルム成形性が良好であつて
好ましい。なお、線状低密度ポリエチレンには酸
化防止剤、スリツプ剤、アンチブロツク剤などの
添加剤が含まれていてもよい。
本発明における線状低密度ポリエチレンに代え
て低密度ポリエチレン、高密度ポリエチレン、エ
チレン−酢酸ビニル共重合体などを使用すると、
エチレン−プロピレンブロツク共重合体との配合
比が適切であれば充分な接着力が得られるもの
の、得られる積層フイルムの透明性およびフイル
ム外観が不良となる。
エチレン−プロピレンブロツク共重合体として
は、結晶性であつて、共重合体中のエチレン含有
量が3〜10重量%、好ましくは5〜8重量%の範
囲のものが使用される。エチレン−プロピレンブ
ロツク共重合体のエチレン含有量が3重量%より
少ない場合はポリエチレン層との接着力が充分得
られず、エチレン含有量が10重量%より多い場合
は、共重合体の製造そのものが困難となるばかり
でなく、ジエルの発生によりフイルム外観が悪化
するため好ましくない。エチレン−プロピレンブ
ロツク共重合体のメルトフローレイシヨは0.5〜
15g/10分のものが好ましい。なお、これらのエ
チレン−プロピレンブロツク共重合体には酸化防
止剤、滑剤、アンチブロツク剤などの添加剤が含
まれていてもよい。
エチレン−プロピレンブロツク共重合体に代え
てプロピレンホモポリマーあるいはエチレン−プ
ロピレンランダム共重合体を使用すると、ポリエ
チレン層との接着力が不充分であるか、あるいは
充分な接着力が得られる場合であつても、積層フ
イルムの透明性およびフイルム外観が劣る。
本発明における接着剤層組成物の組成は、線状
低密度ポリエチレンが40〜60重量%であつてエチ
レン−プロピレンブロツク共重合体が60〜20重量
%であることが必須である。特に線状低密度ポリ
エチレンが50〜70重量%であつてエチレン−プロ
ピレンブロツク共重合体が50〜30重量%であるこ
とが好ましい。線状低密度ポリエチレンが80重量
%を越える場合はポリプロピレン層と接着剤組成
物層とがほとんど接着されず、エチレン−プロピ
レンブロツク共重合体が20重量%未満ではポリプ
ロピレン層とほとんど接着されない。また、エチ
レン−プロピレンブロツク共重合体が60重量%を
越える場合は、透明性およびフイルム外観が不良
となる。
この発明においては、線状低密度ポリエチレン
40〜80重量%とエチレン−プロピレンブロツク共
重合体60〜20重量%とを配合し、そのまま、また
は事前に溶融混練したものを、例えば積層フイル
ム製造装置を用いて、溶融状態のポリエチレン層
とポリプロピレン層との間に介在させて積層し冷
却固化することによつて積層フイルムを製造す
る。
線状低密度ポリエチレンとエチレン−プロピレ
ンブロツク共重合体とを配合する方法は、公知の
あらゆる方法が使用でき、積層フイルム製造装置
の押出機で行つてもよいし、その前に別の押出機
で行つてもよい。
前記の積層フイルム製造装置とは、押出機を3
台以上組合わせて、1個のダイから多層フイルム
を押し出すものであれば、インフレーシヨン法フ
イルム製造装置でも、T−ダイ法フイルム製造装
置でもよい。
前記のポリエチレン層を形成するポリエチレン
層およびポリプロピレン層を形成するポリプロピ
レンとしては、従来フイルム用に使用されている
ポリエチレンおよびポリプロピレンがそれぞれ使
用される。
この発明の方法によつて得られる積層フイルム
は、好ましくはポリエチレン層の厚さが5〜
10μ、接着剤組成物層の厚さが3〜100μ、ポリプ
ロピレン層の厚さが5〜100μであるものが好ま
しい。
〔実施例〕
以下に実施例および比較例を示す。以下の各例
において、部は重量部を意味し、%は重量%を意
味する。
以下の各例において使用したポリエチレンおよ
びポリプロピレンを表示する記号とその内容を以
下に示す。但し、MIはメルトインデツクスを、
MFRはメルトフローレイシヨを、dは密度を表
す。
A:ポリエチレン(宇部興産製)
MI0.8g/10分、d0.922g/cm3、ホモポリマ
ー
B:エチレン−酢酸ビニル共重合体(宇部興産
製)
MI2.0g/10分、酢酸ビニル含有量15%
C:線状低密度ポリエチレン(宇部興産製)
MIg/10分、d0.919g/cm3
:エチレン−プロピレンランダム共重合体(宇
部興産製)
MFR:g/10分、エチレン含有量3.0%
:ポリプロピレン(宇部興産製)
MFR9.0g/10分、ホモポリマー
:エチレン−プロピレンブロツク共重合体(宇
部興産製)
MFR1.0g/10分、エチレン含有量3.0%
:エチレン−プロピレンブロツク共重合体(宇
部興産製)
MFR1.0g/10分、エチレン含有量3.0%
実施例 1〜6
第1表に示す種類のポリエチレンとポリプロピ
レンとを用いて、下記の装置および方法により積
層フイルムを製造した。
3種3層Tダイ成形装置を用い、外層にポリプ
ロピレン、内層にポリエチレン、中間層(接着剤
組成物層)にポリエチレンとポリプロピレンとの
ブレンド物を用いて積層フイルムを製造した。外
層のポリプロピレン層としては前記のポリプロ
ピレン層ポモポリマーを、内層のポリエチレン層
としては前記Aのポリエチレンホモポリマーを用
いた。
製造条件は、外層が180〜220℃、中間層が190
〜200℃、内層が160〜220℃、ダイ温度が250℃で
あり、引取速度は6m/minで行つた。フイルム
厚さは外層が20μ、中間層が10μ、内層が20μであ
る。
こうしてできた積層フイルムの剥離強度および
ヘイズ(透明性)をそれぞれJIS K6854および
JIS Z1702に従つて測定した。結果を第1表に示
す。なお、第1表の剥離強度の値は外層(ポリプ
ロピレン層)と中間層(接着剤層)とを剥離した
時の値である。内層(ポリエチレン層)と中間層
(接着剤層)との間は非常に強固に一体となつて
おり剥離不能であつた。
[Industrial Application Field] The present invention relates to a method for producing a laminated film in which polyethylene and polypropylene are bonded together via an adhesive layer. [Prior art and its problems] Although polyethylene and polypropylene are the same polyolefin, they are hardly compatible with each other.
When made into a laminated film, the mutual adhesion is extremely poor, and the appearance of the film is also not good. For this reason, the applications of laminated films of polyethylene and polypropylene have been significantly limited. Conventionally, attempts have been made to interpose various adhesive layers between both films to improve adhesiveness. However, a laminated film that provides sufficient adhesive strength and has a good film appearance has not yet been developed. [Means for Solving the Problems] The present invention provides a method for producing a laminated film in which a polyethylene layer and a polypropylene layer are bonded sufficiently strongly and which has good transparency and appearance. The present invention comprises linear low density polyethylene of 40 to 80% by weight and ethylene-propylene block copolymer having an ethylene content of 3 to 10% by weight of 60 to 20% by weight.
(hereinafter referred to as adhesive composition)
The present invention relates to a method for producing a laminated film, which comprises interposing the polyethylene layer and the polypropylene layer in a molten state, and then cooling and solidifying the polyethylene layer and the polypropylene layer. The linear low-density polyethylene is ethylene-polyethylene, which is obtained by copolymerizing 50 mol% or more of ethylene and α-olefin by a known method such as solution polymerization, gas phase polymerization, or slurry polymerization using a transition metal catalyst.
Alpha-olefin copolymers may be used. α-olefins used in copolymerization include propylene, butene, pentene, and 4-methylpentene.
1, octene, etc. Linear low-density polyethylene is suitable as a raw material for the ultra-thin adhesive layer film used in the present invention because of its excellent transparency, heat resistance, mechanical strength, etc. The melt index of linear low density polyethylene is 0.5 to 20.
g/10 minutes is preferable because it provides good film formability. The linear low-density polyethylene may contain additives such as antioxidants, slip agents, and anti-blocking agents. When low density polyethylene, high density polyethylene, ethylene-vinyl acetate copolymer, etc. are used in place of linear low density polyethylene in the present invention,
If the blending ratio with the ethylene-propylene block copolymer is appropriate, sufficient adhesive strength can be obtained, but the transparency and appearance of the resulting laminated film will be poor. As the ethylene-propylene block copolymer, one that is crystalline and has an ethylene content in the range of 3 to 10% by weight, preferably 5 to 8% by weight is used. If the ethylene content of the ethylene-propylene block copolymer is less than 3% by weight, sufficient adhesive strength with the polyethylene layer cannot be obtained, and if the ethylene content is more than 10% by weight, the production of the copolymer itself may be affected. This is not preferable because it is not only difficult, but also the appearance of the film deteriorates due to the generation of gel. The melt flow ratio of ethylene-propylene block copolymer is 0.5~
15g/10 minutes is preferred. Incidentally, these ethylene-propylene block copolymers may contain additives such as antioxidants, lubricants, and antiblocking agents. If a propylene homopolymer or an ethylene-propylene random copolymer is used instead of an ethylene-propylene block copolymer, the adhesion to the polyethylene layer may be insufficient, or even if sufficient adhesion can be obtained. Also, the transparency and appearance of the laminated film are poor. In the composition of the adhesive layer composition in the present invention, it is essential that the linear low density polyethylene is 40 to 60% by weight and the ethylene-propylene block copolymer is 60 to 20% by weight. In particular, it is preferable that the linear low density polyethylene is 50 to 70% by weight and the ethylene-propylene block copolymer is 50 to 30% by weight. If the linear low-density polyethylene content exceeds 80% by weight, the polypropylene layer and the adhesive composition layer will hardly be bonded to each other, and if the ethylene-propylene block copolymer content is less than 20% by weight, the polypropylene layer will hardly be bonded to the adhesive composition layer. Furthermore, if the ethylene-propylene block copolymer content exceeds 60% by weight, the transparency and appearance of the film will be poor. In this invention, linear low density polyethylene
A mixture of 40 to 80% by weight of ethylene-propylene block copolymer and 60 to 20% by weight of ethylene-propylene block copolymer is mixed as it is or is melt-kneaded in advance, and then mixed with a molten polyethylene layer and polypropylene using, for example, a laminated film manufacturing device. A laminated film is manufactured by interposing the film between the layers and cooling and solidifying the film. Any known method can be used to blend the linear low-density polyethylene and the ethylene-propylene block copolymer, and it may be carried out using an extruder in the laminated film manufacturing equipment, or it may be blended using a separate extruder before blending. You may go. The above-mentioned laminated film manufacturing equipment includes three extruders.
It may be an inflation method film manufacturing device or a T-die method film manufacturing device as long as it extrudes a multilayer film from one die by combining two or more devices. As the polyethylene layer forming the polyethylene layer and the polypropylene forming the polypropylene layer, polyethylene and polypropylene, which are conventionally used for films, are used, respectively. In the laminated film obtained by the method of this invention, the thickness of the polyethylene layer is preferably 5 to 5.
10μ, the thickness of the adhesive composition layer is preferably 3 to 100μ, and the thickness of the polypropylene layer is preferably 5 to 100μ. [Example] Examples and comparative examples are shown below. In each of the following examples, parts mean parts by weight and % mean % by weight. The symbols representing polyethylene and polypropylene used in each of the following examples and their contents are shown below. However, MI uses melt index,
MFR represents melt flow ratio, and d represents density. A: Polyethylene (manufactured by Ube Industries) MI 0.8 g/10 min, d 0.922 g/cm 3 , homopolymer B: Ethylene-vinyl acetate copolymer (manufactured by Ube Industries) MI 2.0 g/10 min, vinyl acetate content 15 % C: Linear low density polyethylene (manufactured by Ube Industries) MIg/10 minutes, d0.919g/cm 3 : Ethylene-propylene random copolymer (manufactured by Ube Industries) MFR: g/10 minutes, ethylene content 3.0%: Polypropylene (manufactured by Ube Industries) MFR9.0g/10 minutes, homopolymer: ethylene-propylene block copolymer (manufactured by Ube Industries) MFR1.0g/10 minutes, ethylene content 3.0%: ethylene-propylene block copolymer (manufactured by Ube Industries) (manufactured by Kosan) MFR 1.0 g/10 minutes, ethylene content 3.0% Examples 1 to 6 Laminated films were manufactured using the types of polyethylene and polypropylene shown in Table 1 by the following apparatus and method. A laminated film was produced using a three-layer, three-layer T-die molding apparatus using polypropylene for the outer layer, polyethylene for the inner layer, and a blend of polyethylene and polypropylene for the intermediate layer (adhesive composition layer). The polypropylene layer pomopolymer described above was used as the outer polypropylene layer, and the polyethylene homopolymer A described above was used as the inner polyethylene layer. The manufacturing conditions are 180-220℃ for the outer layer and 190℃ for the middle layer.
-200°C, inner layer temperature was 160-220°C, die temperature was 250°C, and take-off speed was 6 m/min. The film thickness is 20μ for the outer layer, 10μ for the middle layer, and 20μ for the inner layer. The peel strength and haze (transparency) of the laminated film thus made were determined according to JIS K6854 and
Measured according to JIS Z1702. The results are shown in Table 1. The peel strength values in Table 1 are the values when the outer layer (polypropylene layer) and the intermediate layer (adhesive layer) are peeled off. The inner layer (polyethylene layer) and intermediate layer (adhesive layer) were very strongly integrated and could not be separated.
【表】
比較例 1〜5
接着剤組成物層を第2表に示す種類の接着剤層
に変えて、実施例1と同じ積層フイルム製造装置
を用い、同じ製造条件で積層フイルムを製造し
た。結果を第2表に示す。[Table] Comparative Examples 1 to 5 Laminated films were manufactured using the same laminated film manufacturing apparatus as in Example 1 under the same manufacturing conditions except that the adhesive composition layer was changed to the type of adhesive layer shown in Table 2. The results are shown in Table 2.
本発明による線状低密度ポリエチレンと特定の
エチレン−プロピレンブロツク共重合体とからな
る接着剤組成物を中間層として用いて、ポリエチ
レン層とポリプロピレン層とを積層した場合、そ
の各層間の接着力は充分であつて、また、各層の
界面における相溶性が良好であるため、積層フイ
ルムの透明性(ヘイズ)およびフイルム外観が非
常に優れている。本発明で得られる積層フイルム
は食品等の包装用フイルムとして好適に使用し得
る。
When a polyethylene layer and a polypropylene layer are laminated using the adhesive composition of the present invention made of linear low-density polyethylene and a specific ethylene-propylene block copolymer as an intermediate layer, the adhesive strength between each layer is This is sufficient, and since the compatibility at the interface between each layer is good, the transparency (haze) of the laminated film and the appearance of the film are excellent. The laminated film obtained by the present invention can be suitably used as a packaging film for foods and the like.
Claims (1)
レン含有量が3〜10重量%の範囲のエチレン−プ
ロピレンブロツク共重合体60〜20重量%とを配合
した組成物の層を、溶融状態のポリエチレン層と
ポリプロピレン層との間に介在させて積層し冷却
固化することを特徴とする積層フイルムの製造方
法。1. A layer of a composition containing 40 to 80% by weight of linear low density polyethylene and 60 to 20% by weight of an ethylene-propylene block copolymer having an ethylene content of 3 to 10% by weight is added to a layer of molten polyethylene. 1. A method for producing a laminated film, which comprises laminating a polypropylene layer and a polypropylene layer, and cooling and solidifying the laminated film.
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
JP15230085A JPS6213338A (en) | 1985-07-12 | 1985-07-12 | Manufacture of laminated film |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
JP15230085A JPS6213338A (en) | 1985-07-12 | 1985-07-12 | Manufacture of laminated film |
Publications (2)
Publication Number | Publication Date |
---|---|
JPS6213338A JPS6213338A (en) | 1987-01-22 |
JPH0331348B2 true JPH0331348B2 (en) | 1991-05-02 |
Family
ID=15537507
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
JP15230085A Granted JPS6213338A (en) | 1985-07-12 | 1985-07-12 | Manufacture of laminated film |
Country Status (1)
Country | Link |
---|---|
JP (1) | JPS6213338A (en) |
Families Citing this family (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DK170114B1 (en) * | 1993-05-05 | 1995-05-29 | Raackmanns Fab As | Bag packaging made of flexible packaging material and method of making it |
JP2005067736A (en) * | 2003-08-05 | 2005-03-17 | Dainippon Printing Co Ltd | Film for packaging cut rice cake |
-
1985
- 1985-07-12 JP JP15230085A patent/JPS6213338A/en active Granted
Also Published As
Publication number | Publication date |
---|---|
JPS6213338A (en) | 1987-01-22 |
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