JPH06339921A - Conductive resin molded product - Google Patents

Conductive resin molded product

Info

Publication number
JPH06339921A
JPH06339921A JP34145293A JP34145293A JPH06339921A JP H06339921 A JPH06339921 A JP H06339921A JP 34145293 A JP34145293 A JP 34145293A JP 34145293 A JP34145293 A JP 34145293A JP H06339921 A JPH06339921 A JP H06339921A
Authority
JP
Japan
Prior art keywords
metal
melting point
thermoplastic resin
conductive
low
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
JP34145293A
Other languages
Japanese (ja)
Other versions
JPH0763970B2 (en
Inventor
Hidehiro Iwase
英裕 岩瀬
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.)
Kyocera Chemical Corp
Original Assignee
Toshiba Chemical Corp
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 Toshiba Chemical Corp filed Critical Toshiba Chemical Corp
Priority to JP34145293A priority Critical patent/JPH0763970B2/en
Publication of JPH06339921A publication Critical patent/JPH06339921A/en
Publication of JPH0763970B2 publication Critical patent/JPH0763970B2/en
Anticipated expiration legal-status Critical
Expired - Fee Related legal-status Critical Current

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  • Injection Moulding Of Plastics Or The Like (AREA)
  • Shielding Devices Or Components To Electric Or Magnetic Fields (AREA)
  • Reinforced Plastic Materials (AREA)
  • Processing And Handling Of Plastics And Other Materials For Molding In General (AREA)

Abstract

PURPOSE:To prevent the deterioration of the conductivity of a molded product even at high temp. by subjecting a conductive resin compsn. wherein a master pellet obtained by integrally applying and forming a thermoplastic resin layer to the surface of a conductive filler consisting of a copper fiber and a low m.p. metal is compounded with a thermoplastic resin pellet to injection molding at a temp. equal to or higher than the m.p. of the low m.p. metal. CONSTITUTION:A conductive resin compsn. wherein a master pellet obtained by integrally applying and forming a thermoplastic resin layer (C) (e.g; polypropylene resin) to the surface of a conductive filler consisting of a copper fiber (A) and a low m.p. metal (B) (e.g; tin) is compounded with a thermoplastic resin pellet (D) is subjected to injection molding at a temp. equal to or higher than the m.p. of the low m.p. metal. The obtained conductive resin molded product generates no separation and scattering of the low m.p. metal at the time of molding processing and does not lower in its conductivity even when a high temp. environmental change is applied and is excellent in the stability of electromagnetic wave shielding effect with the elapse of time. When the molded product is used in electronic machinery or communication machinery, extremely high reliability can be imparted.

Description

【発明の詳細な説明】Detailed Description of the Invention

【0001】[0001]

【産業上の利用分野】本発明は、導電性、特にその経時
安定性に優れた、信頼性の高い導電性樹脂成形品に関す
る。
BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a highly reliable conductive resin molded article having excellent conductivity, especially stability over time.

【0002】[0002]

【従来の技術】従来より、熱可塑性樹脂に導電性繊維を
配合して導電性樹脂組成物とし、該組成物は導電性樹脂
成形品の材料に利用されてきた。これらには主に炭素系
の導電性繊維が配合されてきたが、その用途は静電気防
止が主で、近年問題になっている電磁波シールドに対し
ては導電性が低くあまり有効でない。そこで電磁波シー
ルド用には金属系の導電性繊維(以下単に金属繊維とい
う)を使用して導電性を向上させることが行われてい
る。
2. Description of the Related Art Conventionally, a conductive resin is blended with a thermoplastic resin to form a conductive resin composition, which has been used as a material for a conductive resin molded article. Carbon-based conductive fibers have been mainly blended with these, but their use is mainly for the prevention of static electricity, and they have low conductivity and are not very effective for the electromagnetic wave shield which has become a problem in recent years. Therefore, for electromagnetic wave shielding, metal-based conductive fibers (hereinafter simply referred to as metal fibers) are used to improve conductivity.

【0003】しかし、金属繊維を配合すると比重が大き
くなり、また樹脂がもつ本来の特性を大きく損なうとい
う問題があり、その配合量を最小限にすることが要求さ
れている。ところが、これらの金属繊維の配合量を減少
させると、導電性が低下し、更には使用環境についても
大きな制約を受ける。すなわち、使用する樹脂と金属繊
維との熱膨張の差により、高温になると導電性が劣化す
るという問題が生ずる。そのため、現状では金属繊維の
配合量を多くして導電性の低下・劣化を防止し、かつ使
用環境を限定することによって実用化されている。その
ように従来の金属繊維の導電性樹脂組成物及び成形品は
用途に制約を受け、かつ特性が不安定で信頼性も低いと
いう問題点があった。
However, when the metal fibers are blended, the specific gravity becomes large, and the original characteristics of the resin are greatly impaired, and it is required to minimize the blending amount. However, if the blending amount of these metal fibers is reduced, the conductivity is lowered, and further the use environment is greatly restricted. That is, due to the difference in thermal expansion between the resin used and the metal fiber, there arises a problem that the conductivity deteriorates at high temperatures. Therefore, at present, it has been put to practical use by increasing the blending amount of metal fibers to prevent the deterioration / deterioration of conductivity and limiting the use environment. As described above, the conventional conductive resin composition of metal fibers and molded products have the problems that their applications are restricted, their characteristics are unstable, and their reliability is low.

【0004】また低融点金属と熱可塑性樹脂とを混合す
ることにより導電性の得られることが知られているが、
低融点金属は樹脂との密着性が悪く、樹脂から分離して
樹脂の物性を低下させ、また成形機の材料色替えの際に
空打等で樹脂と低融点金属とが分離し、金属のみが飛散
する等の成形加工上きわめて危険であるなどの問題があ
った。
It is known that conductivity can be obtained by mixing a low melting point metal and a thermoplastic resin.
The low melting point metal has poor adhesion with the resin and separates from the resin to deteriorate the physical properties of the resin. Moreover, when the color of the material of the molding machine is changed, the resin and the low melting point metal are separated by blanking, etc. However, there is a problem in that it is extremely dangerous in the molding process, such as scatter.

【0005】[0005]

【発明が解決しようとする課題】本発明は、上記問題点
を解決するためになされたもので、高温においても成形
品の導電性が劣化せず、特にその経時安定性に優れ、成
形加工時においても樹脂低融点金属との分離、飛散など
がなく、成形加工性のよい、信頼性の高い導電性樹脂成
形品を提供しようとするものである。
SUMMARY OF THE INVENTION The present invention has been made in order to solve the above-mentioned problems, and the conductivity of a molded product does not deteriorate even at high temperatures, and in particular, its stability with time is excellent, and during molding processing. Also in the above, there is a need to provide a highly reliable conductive resin molded product which is free from separation and scattering of a resin having a low melting point and has good moldability.

【0006】[0006]

【課題を解決するための手段】本発明者は、上記の目的
を達成しようと鋭意研究を重ねた結果、導電性充填材と
して、銅繊維と、通常熱可塑性樹脂より高い融点を有す
る低融点金属とを併用することによって、高温において
も成形品の導電性の劣化がなく、成形加工時においても
熱可塑性樹脂と低融点金属との分離・飛散のない導電性
樹脂成形品が得られることを見いだし本発明を完成した
ものである。
Means for Solving the Problems As a result of intensive studies aimed at achieving the above-mentioned object, the present inventor has found that copper fibers as a conductive filler and a low melting point metal having a melting point higher than that of a thermoplastic resin are usually used. It was found that the combined use of and makes it possible to obtain a conductive resin molded product in which the conductivity of the molded product does not deteriorate even at high temperatures and the thermoplastic resin and the low melting point metal do not separate or scatter during molding. The present invention has been completed.

【0007】すなわち、本発明は、(A)銅繊維及び
(B)低融点金属からなる導電性充填材の表面に(C)
熱可塑性樹脂層を被覆形成一体化したペレット状のマス
ターペレットと、(D)熱可塑性樹脂ペレットとを配合
した導電性樹脂組成物を、低融点金属の融点以上の温度
で射出成形してなることを特徴とする導電性樹脂成形品
である。
That is, according to the present invention, (C) is formed on the surface of a conductive filler composed of (A) copper fiber and (B) low melting point metal.
A conductive resin composition prepared by blending a pellet-shaped master pellet in which a thermoplastic resin layer is integrally formed by coating and (D) a thermoplastic resin pellet is injection-molded at a temperature equal to or higher than the melting point of a low-melting metal. Is a conductive resin molded product.

【0008】本発明に用いる(A)銅繊維としては、長
繊維状の銅繊維、銅層を有する有機繊維、炭素繊維など
が挙げられる。銅繊維の直径は5 〜100 μm 程度のもの
が望ましく、この銅繊維は、後述する(B)低融点金属
と集合させて導電性充填材とし、次いで(C)熱可塑性
樹脂層で被覆形成一体化し、長さ5 〜8mm に切断してマ
スターペレットとする。銅繊維の含有量は、全体の導電
性組成物に対して0.5〜30重量%含有することが望まし
い。0.5 重量%未満では導電性が低く、また30重量%を
超えると組成物の流動性や物性が低下し好ましくない。
Examples of the copper fiber (A) used in the present invention include long fiber copper fibers, organic fibers having a copper layer, and carbon fibers. It is desirable that the diameter of the copper fiber is about 5 to 100 μm. The copper fiber is aggregated with a low melting point metal (B) to be described later to form a conductive filler, and then (C) a thermoplastic resin layer to form a coating. And cut it to a length of 5 to 8 mm to make a master pellet. The content of the copper fibers is preferably 0.5 to 30% by weight based on the whole conductive composition. If it is less than 0.5% by weight, the conductivity is low, and if it exceeds 30% by weight, the fluidity and physical properties of the composition are deteriorated, which is not preferable.

【0009】本発明に用いる(B)低融点金属としては
Sn 又はSn −Pb を主成分とする一般のハンダ合金、
Sn −Pb −Ag を主成分とする高温ハンダ合金、さら
にはSn −Pb −Bi を主成分とする低温ハンダ合金等
が挙げられる。低融点金属は、繊維状、線状、棒状、そ
のいずれでもよく、特にその形状に限定されるものでは
ない。前述の銅繊維はこの低融点金属と集合させるが、
銅繊維と繊維状の低融点金属とを単に集合させても、銅
繊維の表面に低融点金属の層を形成したものでもよい。
また、銅繊維に粒状の低融点金属をサイジングしてもよ
く、その集合の方法を限定するものではない。こうして
銅繊維と低融点金属とからなる導電性充填材をつくる。
これらの低融点金属の融点は、混合する熱可塑性樹脂の
成形加工温度によって選定すること、すなわち、熱可塑
性樹脂の融点より高い融点を有することが望ましく、そ
のような低融点金属を選定使用することである。低融点
金属の含有量は銅繊維に対して5 〜30重量%含有するこ
とが望ましい。その含有量が5 重量%未満では銅繊維を
結合、被覆することが不充分となり、また30重量%を超
えると過剰の低融点金属が遊離して、組成物の物性を低
下させ好ましくない。
As the low melting point metal (B) used in the present invention, a general solder alloy containing Sn or Sn-Pb as a main component,
Examples thereof include a high temperature solder alloy containing Sn-Pb-Ag as a main component, and a low temperature solder alloy containing Sn-Pb-Bi as a main component. The low melting point metal may be fibrous, linear or rod-shaped, and is not particularly limited to the shape. The above-mentioned copper fiber is assembled with this low melting point metal,
The copper fiber and the fibrous low melting point metal may be simply aggregated, or the layer of the low melting point metal may be formed on the surface of the copper fiber.
The granular low melting point metal may be sized on the copper fiber, and the method of assembling the metal is not limited. Thus, a conductive filler made of copper fibers and a low melting point metal is prepared.
The melting point of these low melting point metals should be selected according to the molding processing temperature of the thermoplastic resin to be mixed, that is, it is desirable to have a melting point higher than the melting point of the thermoplastic resin, and such low melting point metals should be selected and used. Is. The content of the low melting point metal is preferably 5 to 30% by weight based on the copper fiber. If the content is less than 5% by weight, binding and coating of copper fibers will be insufficient, and if it exceeds 30% by weight, excessive low melting point metal will be liberated and the physical properties of the composition will be deteriorated, such being undesirable.

【0010】本発明で(C)熱可塑性樹脂層を形成する
ものとしては、ポリプロピレン樹脂、ポリエチレン樹
脂、ポリスチレン樹脂、アクリロニトリル・ブタジエン
・スチレン樹脂、変性ポリフェニレンオキサイド樹脂、
ポリブチレンテレフタレート樹脂、ポリカーボネート樹
脂、ポリアミド樹脂、ポリエーテルイミド樹脂等が挙げ
られる。この熱可塑性樹脂は、銅繊維と低融点金属とを
被覆するものである。
In the present invention, the (C) thermoplastic resin layer is formed by polypropylene resin, polyethylene resin, polystyrene resin, acrylonitrile butadiene styrene resin, modified polyphenylene oxide resin,
Examples thereof include polybutylene terephthalate resin, polycarbonate resin, polyamide resin, and polyetherimide resin. This thermoplastic resin coats the copper fibers and the low melting point metal.

【0011】本発明に用いる(D)熱可塑性樹脂ペレッ
ト(以下ナチュラルペレットという)は、前記の(C)
熱可塑性樹脂層と同種又は同一のものでもよい。また
(C)の熱可塑性樹脂層と混合されることによって界面
に形成される第三の合成樹脂が補強効果をもつもの、す
なわちブレンドポリマーとなるものでもよい、例えば、
(C)熱可塑性樹脂層として変性PPO樹脂、ポリカー
ボネート樹脂等を使用するときはナチュラルペレットと
してスチレン系の熱可塑性樹脂を使用すると好結果が得
られる。こうすることによっり界面に形成される第三の
合成樹脂が補強効果をもつものである。これらの組合せ
を用いることによって、特性の優れた成形品を得ること
ができる。
The thermoplastic resin pellets (D) used in the present invention (hereinafter referred to as natural pellets) are the same as the above-mentioned (C).
It may be the same as or the same as the thermoplastic resin layer. Further, the third synthetic resin formed at the interface by being mixed with the thermoplastic resin layer (C) may have a reinforcing effect, that is, a blended polymer, for example,
(C) When using a modified PPO resin, a polycarbonate resin, or the like as the thermoplastic resin layer, good results can be obtained by using a styrene-based thermoplastic resin as the natural pellets. By doing so, the third synthetic resin formed on the interface has a reinforcing effect. By using these combinations, a molded article having excellent properties can be obtained.

【0012】本発明の導電性樹脂成形品は、通常次のよ
うにして製造することができる。長繊維状の銅繊維と、
低融点金属とを集合させて導電性充填材とし、押出機の
ダイスを通して導電性充填材の表面に熱可塑性樹脂層を
被覆形成し、次いで適当な大きさに切断してペレット状
にしてマスターペレットとする。マスターペレットは通
常断面が円形であるが、円形でなくとも偏平、その他の
形状でもよく特に形状に制限されない。また、マスター
ペレットの製造工程は連続的に行うことが経済的に有利
であるが、必ずしも連続的でなくともバッチ方式で製造
してもよい。このマスターペレットに熱可塑性樹脂のみ
からなるナチュラルペレットを配合して導電性樹脂組成
物とする。配合するナチュラルペレットは、導電性樹脂
組成物やその成形品に要求される特性に応じて、熱可塑
性樹脂およびその量が適切に選択される。
The conductive resin molded article of the present invention can be usually manufactured as follows. Long fiber copper fiber,
A low melting point metal is aggregated to form a conductive filler, a thermoplastic resin layer is formed on the surface of the conductive filler through a die of an extruder, and then cut into an appropriate size to form a pellet, which is a master pellet. And The master pellet usually has a circular cross section, but the shape is not limited to a flat shape and may be any shape other than the circular shape. Further, although it is economically advantageous to carry out the manufacturing process of the master pellet continuously, the master pellet may not necessarily be manufactured continuously but may be manufactured by a batch method. This master pellet is blended with a natural pellet made of only a thermoplastic resin to prepare a conductive resin composition. For the natural pellets to be blended, the thermoplastic resin and the amount thereof are appropriately selected according to the properties required for the conductive resin composition and its molded product.

【0013】こうして製造された導電性樹脂組成物を低
融点金属の融点以上の温度で射出成形して、本発明の導
電性樹脂成形品とすることができる。本発明の導電性樹
脂成形品は、電磁波シールドを必要とする電子機器、計
測機器、通信機器等のハウジングや部品に使用して好適
である。
The conductive resin composition thus produced can be injection-molded at a temperature not lower than the melting point of the low melting point metal to obtain the conductive resin molded article of the present invention. The conductive resin molded product of the present invention is suitable for use in housings and parts of electronic devices, measuring devices, communication devices and the like that require electromagnetic wave shielding.

【0014】[0014]

【作用】本発明によれば、導電性充填材として銅繊維と
低融点金属を併用したことによって、銅繊維間の接合点
を低融点金属が融着して強固な網目状の結合を形成し、
その結果、導電性の劣化がなくなる。従って、銅繊維配
合量の減少が可能となり、樹脂本来の特性を損なうこと
もない。また熱可塑性樹脂の成形加工温度によって溶融
する低融点金属を選択し、銅繊維と強固に融着するた
め、低融点金属の分離や飛散等がない。
According to the present invention, by using the copper fiber and the low melting point metal together as the conductive filler, the low melting point metal is fused at the joining point between the copper fibers to form a strong mesh-like bond. ,
As a result, the conductivity is not deteriorated. Therefore, it becomes possible to reduce the amount of copper fiber compounded, and the original characteristics of the resin are not impaired. Further, since a low melting point metal that melts depending on the molding processing temperature of the thermoplastic resin is selected and firmly fused with the copper fiber, there is no separation or scattering of the low melting point metal.

【0015】[0015]

【実施例】次に本発明を実施例によって説明する。EXAMPLES The present invention will now be described with reference to examples.

【0016】実施例 直径50μm の銅繊維を300 本収束し、この銅繊維に直径
300 μm の繊維状の低融点金属(Sn 60%、Pb 40%)
を集合させて束ねて導電性充填材とし、タフレックス4
10(三菱モンサント化成社製、ABS樹脂、商品名)
を用いて押出機のダイスを通し、導電性充填材の表面に
ABS樹脂を溶融被覆した。これを冷却してペレタイザ
ーで繊維方向に6mm の長さに切断してマスターペレット
とした。このマスターペレットに、タフレックス410
(前出)のナチュラルペレットを配合して導電性樹脂組
成物を製造した。この場合の銅繊維の充填率は30重量%
であった。この導電性樹脂組成物を用いて、射出成形を
行い成形品を得た。成形品について体積抵抗率、シール
ド効果の試験を行ったのでその結果を表1に示したが、
本発明の極めて顕著な効果が確認された。
Example 300 300 copper fibers each having a diameter of 50 μm were converged, and the copper fibers were
300 μm fibrous low melting point metal (Sn 60%, Pb 40%)
Tufflex 4 by collecting and bundling them as a conductive filler
10 (Made by Mitsubishi Monsanto Kasei Co., ABS resin, trade name)
Was passed through a die of an extruder to melt-coat the surface of the conductive filler with ABS resin. This was cooled and cut into a length of 6 mm in the fiber direction with a pelletizer to obtain master pellets. Tough Rex 410 is added to this master pellet.
A conductive resin composition was produced by blending the natural pellets (described above). The filling rate of copper fiber in this case is 30% by weight
Met. Injection molding was performed using this conductive resin composition to obtain a molded product. The molded products were tested for volume resistivity and shielding effect. The results are shown in Table 1.
The extremely remarkable effect of the present invention was confirmed.

【0017】比較例 実施例において低融点金属を用いない以外はすべて実施
例と同一にしてマスターペレット、導電性樹脂組成物お
よび成形品をつくり、その成形品について実施例と同様
に試験を行ったのでその結果を表1に示した。
Comparative Example A master pellet, a conductive resin composition and a molded product were prepared in the same manner as in the Example except that the low melting point metal was not used, and the molded product was tested in the same manner as in the Example. The results are shown in Table 1.

【0018】[0018]

【表1】 [Table 1]

【0019】[0019]

【発明の効果】以上の説明および表1からも明らかなよ
うに、本発明の導電性樹脂成形品は、導電性充填材とし
て銅繊維と低融点金属を併用したことによって、銅繊維
同士の結合が強固となり、銅繊維の配合量を減少でき、
また成形加工時における低融点金属の分離・飛散がなく
成形加工性が向上した。また本発明の成形品は、高温に
おける環境変化を加えても導電性が低下することなく、
電磁波シールド効果の経時安定性に優れたものである。
この成形品を電子機器、通信機器等に使用すれば極めて
高い信頼性を付与することができる。
As is clear from the above description and Table 1, the conductive resin molded article of the present invention uses copper fibers and a low melting point metal together as the conductive filler to bond the copper fibers together. Becomes stronger, the amount of copper fiber compounded can be reduced,
In addition, there was no separation and scattering of the low melting point metal during the molding process, improving the moldability. Further, the molded article of the present invention, the conductivity does not decrease even when subjected to environmental changes at high temperatures,
The electromagnetic wave shielding effect is excellent in stability over time.
If this molded product is used in electronic devices, communication devices, etc., extremely high reliability can be imparted.

───────────────────────────────────────────────────── フロントページの続き (51)Int.Cl.5 識別記号 庁内整理番号 FI 技術表示箇所 H05K 9/00 W // B29K 105:16 ─────────────────────────────────────────────────── ─── Continuation of the front page (51) Int.Cl. 5 Identification code Office reference number FI technical display location H05K 9/00 W // B29K 105: 16

Claims (1)

【特許請求の範囲】[Claims] 【請求項1】 (A)銅繊維及び(B)低融点金属から
なる導電性充填材の表面に(C)熱可塑性樹脂層を被覆
形成一体化したペレット状のマスターペレットと、
(D)熱可塑性樹脂ペレットとを配合した導電性樹脂組
成物を、低融点金属の融点以上の温度で射出成形してな
ることを特徴とする導電性樹脂成形品。
1. A pellet-shaped master pellet in which (C) a thermoplastic resin layer is coated and integrated on the surface of a conductive filler composed of (A) copper fibers and (B) a low melting point metal,
(D) A conductive resin molded article obtained by injection-molding a conductive resin composition containing a thermoplastic resin pellet at a temperature equal to or higher than the melting point of a low melting point metal.
JP34145293A 1993-12-10 1993-12-10 Conductive resin molding Expired - Fee Related JPH0763970B2 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP34145293A JPH0763970B2 (en) 1993-12-10 1993-12-10 Conductive resin molding

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP34145293A JPH0763970B2 (en) 1993-12-10 1993-12-10 Conductive resin molding

Related Parent Applications (1)

Application Number Title Priority Date Filing Date
JP5199887A Division JPH0647254B2 (en) 1987-03-09 1987-03-09 Conductive resin composition

Publications (2)

Publication Number Publication Date
JPH06339921A true JPH06339921A (en) 1994-12-13
JPH0763970B2 JPH0763970B2 (en) 1995-07-12

Family

ID=18346188

Family Applications (1)

Application Number Title Priority Date Filing Date
JP34145293A Expired - Fee Related JPH0763970B2 (en) 1993-12-10 1993-12-10 Conductive resin molding

Country Status (1)

Country Link
JP (1) JPH0763970B2 (en)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2007154015A (en) * 2005-12-05 2007-06-21 Sumitomo Chemical Co Ltd Process for producing molded article made of electroconductive thermoplastic resin
JP2008537916A (en) * 2005-04-13 2008-10-02 クール オプションズ,インコーポレーテッド In-mold metallized polymer component and method for producing the same

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2008537916A (en) * 2005-04-13 2008-10-02 クール オプションズ,インコーポレーテッド In-mold metallized polymer component and method for producing the same
JP2007154015A (en) * 2005-12-05 2007-06-21 Sumitomo Chemical Co Ltd Process for producing molded article made of electroconductive thermoplastic resin

Also Published As

Publication number Publication date
JPH0763970B2 (en) 1995-07-12

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