JPS63242626A - Biaxially oriented poly-p-phenylenesulfide film - Google Patents

Biaxially oriented poly-p-phenylenesulfide film

Info

Publication number
JPS63242626A
JPS63242626A JP7835887A JP7835887A JPS63242626A JP S63242626 A JPS63242626 A JP S63242626A JP 7835887 A JP7835887 A JP 7835887A JP 7835887 A JP7835887 A JP 7835887A JP S63242626 A JPS63242626 A JP S63242626A
Authority
JP
Japan
Prior art keywords
film
haze
biaxially oriented
oriented poly
inorganic particles
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.)
Granted
Application number
JP7835887A
Other languages
Japanese (ja)
Other versions
JPH048456B2 (en
Inventor
Yukio Noguchi
幸男 野口
Masaaki Sudo
正昭 須藤
Yukichi Deguchi
出口 雄吉
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Toray Industries Inc
Original Assignee
Toray Industries Inc
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Toray Industries Inc filed Critical Toray Industries Inc
Priority to JP7835887A priority Critical patent/JPS63242626A/en
Publication of JPS63242626A publication Critical patent/JPS63242626A/en
Publication of JPH048456B2 publication Critical patent/JPH048456B2/ja
Granted legal-status Critical Current

Links

Abstract

PURPOSE:To obtain a biaxially oriented poly-p-phenylenesulfide film, which has favorable slip properties and a few bulking projections and insulation defects, by a structure wherein the film contains the specified weight of inactive inorganic particles and has the internal haze per unit thickness and external haze of specified values. CONSTITUTION:The film concerned is a biaxially oriented poly-p- phenylenesulfide film, which contains 0.3-1.5wt.% of inactive inorganic particles and the internal haze per unit thickness of which is 1-3%/mum, and the external haze of which is 5-20%. If the content of the inactive inorganic particle is below 0.3wt.%, the slip properties of the film become poor. If said content exceeds 1.5wt.% insulation defect increases. If the internal haze per unit thickness is below 1%/mum, the slip properties of the film become poor. If said internal haze exceeds 3%/mum, insulation defect increase. If the external haze is below 5%, the slip properties become poor. If said external haze exceeds 20%, the mechanical characteristics of the film become inferior and brittle.

Description

【発明の詳細な説明】 [産業上の利用分野] この発明は、2軸配向ポリ−p−フェニレンスルフィド
フィルムに関する。
DETAILED DESCRIPTION OF THE INVENTION [Industrial Field of Application] This invention relates to biaxially oriented poly-p-phenylene sulfide films.

[従来技術及びその欠点] 2軸配向ポリ−p−フェニレンスルフィドフィルムは、
耐熱性、耐薬品性、電気絶縁性、誘電特性、機械物性等
の点て、極めて優れた性能を有しており、耐熱性電気絶
縁材料として注目されている。
[Prior art and its drawbacks] Biaxially oriented poly-p-phenylene sulfide film is
It has extremely excellent performance in terms of heat resistance, chemical resistance, electrical insulation, dielectric properties, mechanical properties, etc., and is attracting attention as a heat-resistant electrical insulating material.

従来より、2軸配向ポリ−p−フェニレンスルフィトフ
ィルムの性質を改善するために、これに不活性*a粒子
を配合することが知られている。
It has been known that in order to improve the properties of a biaxially oriented poly-p-phenylene sulfite film, inert *a particles are added thereto.

例えば、特開昭55−:14968号には、フィルムの
表面粗度を調整するl的で重合時あるいは重合終了時に
ポリマー中に不活性無機粒子を添加し、又は重合のため
に使用した不溶解塩を一定量残存させることが開示され
ている。また、特開昭60−257510号には、2軸
配向ポリ−p−フェニレンスルフィドフィルムをコンデ
ンサの誘電体として用いた場合に、その容量及び絶縁破
壊電圧のバラツキを小さくするために、微細突起密度及
び粗大突起密度を一定範囲に調整した2軸配向ポリ−p
−フェニレンスルフィトフィルムか開示されており、微
細突起密度及び粗大突起密度を調整するために、必要に
応じて溶融押出し工程以前の任意の段階て、樹脂組成物
中にモ均粒子径が0.1−1.s終−の微粒子を均一に
分散させることが開示されている。さらに、特公昭59
−5101号には、不活性無機粒子を配合し゛てそのI
t!擦係数を0.75以下に抑え、かつその面粗度の平
均を0,09pm15+sm以下に抑えた2軸配向ポリ
−p−フェニレンスルフィドフィルムが開示されている
For example, JP-A-55-14968 discloses that inert inorganic particles are added to the polymer during or at the end of the polymerization to adjust the surface roughness of the film, or that insoluble particles used for the polymerization are added to the polymer to adjust the surface roughness of the film. It is disclosed that a certain amount of salt remains. Furthermore, in JP-A No. 60-257510, when a biaxially oriented poly-p-phenylene sulfide film is used as a dielectric of a capacitor, in order to reduce variations in capacitance and dielectric breakdown voltage, and biaxially oriented poly-p with coarse protrusion density adjusted within a certain range.
- A phenylene sulfite film is disclosed, and in order to adjust the fine protrusion density and the coarse protrusion density, if necessary, at any stage before the melt extrusion process, the average particle size of the resin composition is set to 0. 1-1. It is disclosed that s-terminated fine particles are uniformly dispersed. In addition, the special public
-5101 contains inert inorganic particles and its I
T! A biaxially oriented poly-p-phenylene sulfide film is disclosed that has a friction coefficient of 0.75 or less and an average surface roughness of 0.09 pm15+sm or less.

しかしながら、2軸配向ポリ−p−フェニレンスルフィ
ドフィルムに無機粒子を比較的大量に添加すると、粒子
中の粗大物の混入及び分散不良による粗大粒子のためフ
ィルム中に粗大突起を生じ易く、その部分が絶縁欠陥と
なる。また、無機粒子を添加したポリ−p−フェニレン
スルフィトフィルムは、延伸中に粒子のまわりにボイド
を生じ絶縁欠陥となる。突起密度を上げてフィルムの滑
り性を向上させるために添加量を増やすと、このボイド
のため絶縁欠陥がさらに増大する。さらにまた、無機粒
子の添加量を減らし、1.5重量%以下程度にすると、
一般にはPJm係数が大きくなり、フィルムの取扱が困
難になったり、フィルムをコンデンサの誘電体として用
いた場合には素子巻き後のプレス工程で絶縁欠陥が増大
する。
However, when a relatively large amount of inorganic particles are added to a biaxially oriented poly-p-phenylene sulfide film, coarse protrusions are likely to occur in the film due to the inclusion of coarse substances in the particles and coarse particles due to poor dispersion. This results in an insulation defect. Further, a poly-p-phenylene sulfite film containing inorganic particles generates voids around the particles during stretching, resulting in insulation defects. If the amount added is increased in order to increase the protrusion density and improve the slipperiness of the film, insulation defects will further increase due to these voids. Furthermore, if the amount of inorganic particles added is reduced to about 1.5% by weight or less,
Generally, the PJm coefficient increases, making it difficult to handle the film, and when the film is used as a dielectric for a capacitor, insulation defects increase in the pressing process after winding the element.

[発明が解決しようとする問題点] この発明の目的は、滑り性が良好であるにもかかわらず
粗大突起及び絶縁欠陥が少ない2軸配向ポリ−p−フェ
ニレンスルフィドフィルムを提供することである。
[Problems to be Solved by the Invention] An object of the present invention is to provide a biaxially oriented poly-p-phenylene sulfide film that has good slip properties but has few coarse protrusions and insulation defects.

[問題点を解決するための手段] 本願発明者らは、鋭意研究の結果、フィルムの厚み当り
の内部ヘイズ及び外部へイズを特定の範囲内にすると、
不活性無機粒子の配合量を少なくしても良好な滑り性が
得られることを見出しこの発明を完成した。
[Means for Solving the Problems] As a result of intensive research, the inventors of the present application found that if the internal haze and external haze per film thickness are within a specific range,
This invention was completed by discovering that good slipperiness can be obtained even if the amount of inert inorganic particles is reduced.

すなわち、この発明は、不活性無機粒子を0.3重量%
から1.5重量%含み、その厚み当りの内部へイズか1
%/p園から3%/#L鵬であり、その外部ヘイズが5
%から20%である2軸配向ポリ−p−フェニレンスル
フィドフィルムを提供する。
That is, this invention contains 0.3% by weight of inert inorganic particles.
Contains 1.5% by weight, internal haze per thickness of 1
%/P garden to 3%/#L Peng, and its external haze is 5
% to 20% biaxially oriented poly-p-phenylene sulfide film.

[発明の効果] この発明の2軸配向ポリ−p−フェニレンスルフィトフ
ィルムは、不活性無機粒子の配合量が比較的少ないので
、粗大突起及び絶縁欠陥も少なく、それでいて滑り性が
良好である。この発明のフィルムは滑り性が良好である
ので取扱が容易であり、絶縁欠陥が少ないので、コンデ
ンサの誘電体として用いると優れた性能を発揮する。
[Effects of the Invention] Since the biaxially oriented poly-p-phenylene sulfite film of the present invention has a relatively small amount of inert inorganic particles, it has few coarse protrusions and insulation defects, and has good slip properties. The film of the present invention has good slip properties, making it easy to handle, and has few insulation defects, so it exhibits excellent performance when used as a dielectric material for capacitors.

[発明の具体的説明] この明細書において、ポリ−p−フェニレンスルフィト
とは、繰り返し単位の70モル%以上(好ましくは85
モル%以上)か、−・般式て示される構成中位から成る
重合体を言う、かかる成分が70モル%未満ではポリマ
ーの結晶性。
[Specific Description of the Invention] In this specification, poly-p-phenylene sulfite refers to 70 mol% or more (preferably 85 mol%) of repeating units.
If the content of such components is less than 70 mol %, the polymer will be crystalline.

熱転移温度等が低くなり、得られるフィルムの耐熱性、
寸法安定性及び機械的特性などを損なう。
The heat transition temperature, etc. is lowered, and the heat resistance of the resulting film is improved.
Impairs dimensional stability and mechanical properties.

繰り返し単位の30モル%未満(好ましくは15モル%
未満)であれば、共重合可能なスルフィド結合を含有す
る単位が含まれていても差支えない。このような単位と
して例えば (たたし、Rは−COOH又は−503H,XはCHl ■ −CHx−1−CHt CH2−1又は−〇−を H3 示す) を挙げることかてきる。
Less than 30 mol% (preferably 15 mol%) of repeating units
(less than), there is no problem even if a unit containing a copolymerizable sulfide bond is included. Examples of such units include (R represents -COOH or -503H, X represents CHl -CHx-1-CHt CH2-1 or -〇- as H3).

この発す1の2軸配向ポリ−p−フェニレンスルフィド
フィルムは、不活性無機粒子を0.311!呈%から1
.5重量%、好ましくは0.3重量%から1.2重星%
含む。不活性無機粒子の含有量が0.3重量%未満では
フィルムの滑り性が不良になり、1.5重量%を超える
と絶縁欠陥が増大する。不活性無機粒子の平均粒径は好
ましくは0.ローから5JL11であり、さらに好まし
くは0.05p、mから2延膿である。不活性無機粒子
としてはポリ−p−フエニレンスルフィドと実質的に反
応しないものであるならば、いずれの無機粒子をも用い
ることがてき、例えば、)&酸カルシウム、シリカ、カ
オリン、タルク、硫酸バリウム、アルミナ、酸化亜鉛、
酸化チタン茅な挙げることかできる。
This biaxially oriented poly-p-phenylene sulfide film of 1 contains inert inorganic particles of 0.311! presentation% to 1
.. 5% by weight, preferably 0.3% to 1.2% by weight
include. If the content of inert inorganic particles is less than 0.3% by weight, the slipperiness of the film will be poor, and if it exceeds 1.5% by weight, insulation defects will increase. The average particle size of the inert inorganic particles is preferably 0. It is 5JL11 from low, more preferably 0.05p, m to 2 pus. As the inert inorganic particles, any inorganic particles can be used as long as they do not substantially react with poly-p-phenylene sulfide; for example, calcium chloride, silica, kaolin, talc, sulfuric acid. barium, alumina, zinc oxide,
Titanium oxide can be mentioned.

この発明の2軸配向ポリ−p−フェニレンスルフィドフ
ィルムの厚み当りの内部ヘイズ(内部ヘイズH)/厚み
(ル曹))は1%/終會から3%/終−である。厚み当
りの内部ヘイズか1%/ps未満てはフィルムの滑り性
か不良になり、3%ん1を超えると絶縁欠陥か増大する
The internal haze per thickness of the biaxially oriented poly-p-phenylene sulfide film of the present invention (internal haze H)/thickness (L) is 1%/final to 3%/final. If the internal haze per thickness is less than 1%/ps, the slipperiness of the film will be poor, and if it exceeds 3%/ps, insulation defects will increase.

また、この発明の2軸配向ポリ−p−フェニレンスルフ
ィドフィルムの外部へイズは5%から20%である。外
部へイズとは全ヘイズから内部へイズを差し引いたもの
であり、これが5%未満であると滑り性が不良になり、
20%を超えるとフィルムの機械的特性が劣りもろくな
る。
Further, the external haze of the biaxially oriented poly-p-phenylene sulfide film of the present invention is from 5% to 20%. External haze is the total haze minus internal haze, and if this is less than 5%, the slipperiness will be poor.
If it exceeds 20%, the mechanical properties of the film will be poor and it will become brittle.

フィルムの厚さは0.3μlか6150 M■が好まし
く、さらに好ましくは0.3終■から25終1、より好
ましくは0.S 74mから10μ園である。
The thickness of the film is preferably 0.3 μl or 6150 M, more preferably 0.3 μl to 25 μl, and more preferably 0.3 μl to 25 μl. S 74m to 10μ garden.

フィルムはまた、10重量%未満の他のポリマー、滑剤
、若色剤及び/又は紫外線吸収剤のような他の添加物を
含んでいてもよい。
The film may also contain less than 10% by weight of other additives such as other polymers, lubricants, young agents and/or UV absorbers.

この発明の2軸配向ポリ−p−フェニレンスルフィドフ
ィルムは次のように製造することがてきる。
The biaxially oriented poly-p-phenylene sulfide film of this invention can be produced as follows.

先ず、常法により製造したポリ−p−フェニレンスルフ
ィド樹脂粉末と不活性無機粒子とをL記重量割合で混合
し、この樹脂組成物を例えばエクストルーダに代表され
る押出し機を用いて常法により溶融押出しし、これを冷
却固化して非晶フィルムを得る。この際、所望ならば、
上記樹脂組成物に10重量%未満の他のポリマー、滑剤
、R色剤、紫外線吸収剤等を添加してもよい。
First, poly-p-phenylene sulfide resin powder produced by a conventional method and inert inorganic particles are mixed at a weight ratio of L, and this resin composition is melted by a conventional method using an extruder such as an extruder. This is extruded and solidified by cooling to obtain an amorphous film. At this time, if desired,
Less than 10% by weight of other polymers, lubricants, R colorants, ultraviolet absorbers, etc. may be added to the resin composition.

次に、この非晶フィルムを長手方向(MD)及び幅方向
(TD)に延伸する。延伸は逐次2軸延伸、同時2輌延
伸のいずれによっても行なうことがてきるが、逐次2軸
延伸により行なうことが好ましい。
Next, this amorphous film is stretched in the longitudinal direction (MD) and the transverse direction (TD). Stretching can be carried out by either sequential biaxial stretching or simultaneous two-machine stretching, but sequential biaxial stretching is preferable.

長手方向延伸時のフィルム温度は97°Cから120℃
の範囲が好ましく、100℃から110℃が特に好まし
い。97℃未満では得られるフィルムのすべり性が不足
てあり、120℃を超えると製膜性か悪化する。加熱時
間は0.2秒から20秒が好ましく、0.2秒から10
秒の範囲が特に好ましい。
Film temperature during longitudinal stretching is 97°C to 120°C
The temperature range is preferably from 100°C to 110°C, particularly preferably from 100°C to 110°C. If it is less than 97°C, the resulting film will have insufficient slipperiness, and if it exceeds 120°C, the film formability will deteriorate. The heating time is preferably from 0.2 seconds to 20 seconds, and from 0.2 seconds to 10 seconds.
A range of seconds is particularly preferred.

加熱方法は特に限定されず、加熱ロール、熱風、ラジエ
ーションヒータなど周知の加熱方法のいずれをも採用す
ることがてきる。延伸手段も特に限定はないか、通常、
複数のロールを用いて行なわれる。延伸倍率は特に限定
はないが1例えば3.2倍から4.5倍である。2軸配
向ポリ−p−フェニレンスルフィドフィルムの外部ヘイ
ズは、艮f方向延伸工程における温度及び加熱時間を調
節することによって調節することができ、外部へイズか
L記範囲内に入るようにこれらの条件を31節する。
The heating method is not particularly limited, and any known heating method such as heating rolls, hot air, and radiation heaters can be employed. There are no particular limitations on the stretching method, and it is usually
Performed using multiple rolls. The stretching ratio is not particularly limited, but is 1, for example, from 3.2 times to 4.5 times. The external haze of the biaxially oriented poly-p-phenylene sulfide film can be adjusted by adjusting the temperature and heating time in the f-direction stretching process, and the external haze can be adjusted so that the external haze falls within the range indicated by L. There are 31 conditions.

とができる、延伸倍率は特に限定はないが例えば3.0
倍から3.8倍である。
The stretching ratio is not particularly limited, but for example, 3.0.
It is from 3.8 times to 3.8 times.

次にこのようにして延伸されたフィルムを常法通りに例
えば240°Cから290”Cて1秒から50秒間足長
熱処理し、この発明の2軸延伸ポリ−p−フェニレンス
ルフィトフィルムを得る。
Next, the thus stretched film is heat-treated in a conventional manner at, for example, 240°C to 290''C for 1 to 50 seconds to obtain a biaxially stretched poly-p-phenylene sulfite film of the present invention. .

なお、内部へイズは、不活性無機粒子の添加量、粒径及
びその分散の程度に依存するので、厚み当りの内部へイ
ズがこの発明の範囲内になるようにこれらを上記範囲内
で適宜選択する。
Note that the internal haze depends on the amount of inert inorganic particles added, the particle size, and the degree of dispersion thereof, so these should be adjusted as appropriate within the above range so that the internal haze per thickness is within the range of this invention. select.

[実施例] 次にこの発明の実施例と比較例を示し、この9、rJ′
]の効果を具体的に説明する。
[Example] Next, Examples and Comparative Examples of the present invention will be shown.
] The effect of this will be explained in detail.

各個において、ヘイズ、絶縁欠陥、摩擦係数並びに強度
及び伸度は以下のようにして測定した。
For each piece, haze, insulation defects, coefficient of friction, strength and elongation were measured as follows.

ヘイズ JIS K−6714に準じて測定した。なお、全ヘイ
ズは試験片を大気中で測定し、内部へイズは試験片をテ
トラリン人の石英セル中に浸漬して測定した。また、外
部ヘイズは全ヘイズから内部ヘイズを引いて算出した。
Haze was measured according to JIS K-6714. Incidentally, the total haze was measured by measuring the test piece in the atmosphere, and the internal haze was measured by immersing the test piece in a Tetralin's quartz cell. Moreover, the external haze was calculated by subtracting the internal haze from the total haze.

絶縁欠陥 フィルム表面抵抗が約3オームになるようにアルミニウ
ムを片面蒸着し、金属の鏡面板上に非蒸着面を下にして
置き、金属板と蒸着面間にフィルム厚さ1終1当り15
0vの直流電圧を印加して。
Aluminum is vapor-deposited on one side so that the surface resistance of the insulation defective film is about 3 ohms, and the non-evaporated side is placed on a metal mirror plate facing down, and the film thickness is 15 ohms per end of the film between the metal plate and the vapor-deposited surface.
Apply a DC voltage of 0v.

絶縁破壊した箇所を数え、フィルムの面積l鳳2当りの
数に換算して絶縁欠陥の指標とした。
The number of locations where dielectric breakdown occurred was counted, and the number was converted to the number per area of the film, which was used as an index of insulation defects.

摩擦係数 ASTM D−113948法に準して、フィルム面同
志の静摩擦係数を、20℃、65$RI+の環境下で測
定した。
Coefficient of Friction According to the ASTM D-113948 method, the coefficient of static friction between film surfaces was measured in an environment of 20°C and 65$RI+.

強度、伸度 JIS C−2318法ニテ、20℃、65!R1+ 
ノ環境下”t’測測定た。
Strength and elongation JIS C-2318 method, 20°C, 65! R1+
The "t' measurement was carried out under the following environment.

実施例1、比較例1及び2 平均粒径1.OJLllの炭酸カルシウムをそれぞれo
、t 、 o、s、又は2.0重量%添加したポリ−p
−フェニレンスルフィド組成物を溶融押出しし、キャス
トドラムEて冷却固化し非晶フィルムを得た0次いて、
105℃に加熱したロールに接触させた後2周速の異な
るロール間て長丁方向(MO)に3.6倍延伸し、テン
ターで幅方向(TD)に100℃て3.4倍延伸し、2
60℃て5秒間定長熱処理して厚さ2終朧の2軸配向ポ
リ−p−フェニレンスルフィトフィルムを得た。このフ
ィルムにつき、内部ヘイズ、外部ヘイズ、摩擦係数、絶
縁欠陥を測定した。結果を表1に示す。
Example 1, Comparative Examples 1 and 2 Average particle size 1. OJLll calcium carbonate, respectively.
, t, o, s, or 2.0% by weight added poly-p
- A phenylene sulfide composition was melt-extruded and cooled and solidified in a cast drum E to obtain an amorphous film.
After being brought into contact with rolls heated to 105°C, it was stretched 3.6 times in the machine direction (MO) between rolls with two different circumferential speeds, and stretched 3.4 times in the width direction (TD) at 100°C with a tenter. ,2
A constant length heat treatment was performed at 60° C. for 5 seconds to obtain a biaxially oriented poly-p-phenylene sulfite film having a thickness of 2 mm. This film was measured for internal haze, external haze, coefficient of friction, and insulation defects. The results are shown in Table 1.

実施例1の方法で平均粒径の異なるシリカ1.5重量%
を添加し、内部ヘイズの異なる厚さ3.5ル■のフィル
ムを作製し、その摩擦係数及び  ゛絶縁欠陥を測定し
た。結果を表2に示す。
1.5% by weight of silica with different average particle sizes by the method of Example 1
3.5 µm thick films with different internal hazes were prepared, and their friction coefficients and insulation defects were measured. The results are shown in Table 2.

実施例1の方法で、MD延伸温度を変えて外部ヘイズの
異なる厚さ6に−のフィルムを作製し、その摩擦係数並
びに強度及び伸度を測定した。結果を表3に示す。
By the method of Example 1, films with different external hazes and thicknesses of 6-6 were produced by changing the MD stretching temperature, and their friction coefficients, strength, and elongation were measured. The results are shown in Table 3.

表3Table 3

Claims (1)

【特許請求の範囲】[Claims] 不活性無機粒子を0.3重量%から1.5重量%含み、
その厚み当りの内部ヘイズが1%/μmから3%/μm
であり、その外部ヘイズが5%から20%である2軸配
向ポリ−p−フェニレンスルフィドフィルム。
Contains 0.3% to 1.5% by weight of inert inorganic particles,
Internal haze per thickness is 1%/μm to 3%/μm
A biaxially oriented poly-p-phenylene sulfide film having an external haze of from 5% to 20%.
JP7835887A 1987-03-31 1987-03-31 Biaxially oriented poly-p-phenylenesulfide film Granted JPS63242626A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP7835887A JPS63242626A (en) 1987-03-31 1987-03-31 Biaxially oriented poly-p-phenylenesulfide film

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP7835887A JPS63242626A (en) 1987-03-31 1987-03-31 Biaxially oriented poly-p-phenylenesulfide film

Publications (2)

Publication Number Publication Date
JPS63242626A true JPS63242626A (en) 1988-10-07
JPH048456B2 JPH048456B2 (en) 1992-02-17

Family

ID=13659765

Family Applications (1)

Application Number Title Priority Date Filing Date
JP7835887A Granted JPS63242626A (en) 1987-03-31 1987-03-31 Biaxially oriented poly-p-phenylenesulfide film

Country Status (1)

Country Link
JP (1) JPS63242626A (en)

Also Published As

Publication number Publication date
JPH048456B2 (en) 1992-02-17

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