JPH08316005A - Conductive composite material composition and conductive complex obtained by molding such composition - Google Patents
Conductive composite material composition and conductive complex obtained by molding such compositionInfo
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- JPH08316005A JPH08316005A JP12202795A JP12202795A JPH08316005A JP H08316005 A JPH08316005 A JP H08316005A JP 12202795 A JP12202795 A JP 12202795A JP 12202795 A JP12202795 A JP 12202795A JP H08316005 A JPH08316005 A JP H08316005A
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- conductive composite
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Abstract
Description
【０００１】[0001]
【産業上の利用分野】本発明は、導電性複合材料組成物
と該組成物を成形して得られる導電性複合体に関する。TECHNICAL FIELD The present invention relates to a conductive composite material composition and a conductive composite obtained by molding the composition.
【０００２】[0002]
【従来の技術】従来、重合体と導電性材料からなる導電
性複合体としてのスイッチング素子として、ポリエチレ
ン等のポリオレフィンとカーボンブラック等の導電性粒
子からなる複合体が知られている（米国特許第２，９７
８，６６５号、特開昭５４−１６６９７号、特開昭５５
−７８４０６号）。2. Description of the Related Art Heretofore, a composite composed of a polyolefin such as polyethylene and conductive particles such as carbon black has been known as a switching element as a conductive composite composed of a polymer and a conductive material (US Pat. 2,97
8,665, JP-A-54-16697, JP-A-55
-78406).
【０００３】[0003]
【発明が解決しようとする課題】ポリエチレンとカーボ
ンブラック粒子の導電性複合体からなるスイッチング素
子は、８０〜１４０℃にスイッチング温度（Ｔｓ）を持
ち（特開昭５５−７８４０６号）、実用上適当な温度で
あるが、ジュール熱による導通抵抗の経時変化（特開昭
５５−７８４０６号）や、導通抵抗とスイッチング素子
の抵抗の関係がヒステレシスを示す（特開平２−９２９
６０号、特開平５−２２６１１３号）ために、再現性に
乏しくさらに改善することが必要である。A switching element composed of a conductive composite of polyethylene and carbon black particles has a switching temperature (Ts) of 80 to 140 ° C. (JP-A-55-78406) and is suitable for practical use. However, the change in conduction resistance due to Joule heat over time (Japanese Patent Laid-Open No. 55-78406) and the relationship between the conduction resistance and the resistance of the switching element show hysteresis (Japanese Patent Laid-Open No. 2-929).
60, JP-A-5-226113), the reproducibility is poor and further improvement is required.
【０００４】本発明の目的は、上記の欠点を改良した再
現性に優れる導電性複合材料組成物と、これを成形して
得られる導電性複合体を提供することにある。An object of the present invention is to provide a conductive composite material composition which has improved the above-mentioned drawbacks and is excellent in reproducibility, and a conductive composite obtained by molding the same.
【０００５】[0005]
【課題を解決するための手段】すなわち本発明は、エチ
レンとプロピレンのランダム共重合体とホモポリプロピ
レンとが直接重合して得られる熱可塑性エラストマーを
含む重合体と、導電性材料からなる導電性複合材料組成
物であって、該重合体１００重量部に対して導電性材料
が２０〜１０００重量部含まれることを特徴とする導電
性複合材料組成物と該組成物を成形して得られる導電性
複合体に関する。Means for Solving the Problems That is, the present invention provides a conductive composite composed of a polymer containing a thermoplastic elastomer obtained by directly polymerizing a random copolymer of ethylene and propylene and homopolypropylene, and a conductive material. A material composition, wherein the conductive material is contained in an amount of 20 to 1000 parts by weight with respect to 100 parts by weight of the polymer, and a conductive material obtained by molding the composition. Regarding the complex.
【０００６】以下本発明を詳細に説明する。本発明にお
けるエチレンとプロピレンのランダム共重合体とホモポ
リプロピレン（以下、ホモＰＰと記載する）とが直接重
合して得られる熱可塑性エラストマーとは、ホモＰＰ部
分が１〜６０重量％で、エチレン成分は１０〜４０重量
％の範囲の重合体であるが、特に限定するものではな
い。また、該重合体の主な特性としてＭＦＲ（Melt Flo
w Rate) 、軟化点等が挙げられる。このうち、ＭＦＲ
（JISK7210) は０．２〜５０g/10分で、好ましくは１．
０〜２０g/10分である。一方、融点（ＤＳＣ法）は、一
般的には１３５〜１７０℃の範囲であり、好ましくは１
４０〜１５５℃である。Hereinafter, the present invention will be described in detail. The thermoplastic elastomer obtained by directly polymerizing a random copolymer of ethylene and propylene in the present invention and homopolypropylene (hereinafter referred to as homoPP) has a homoPP portion of 1 to 60% by weight and an ethylene component. Is a polymer in the range of 10 to 40% by weight, but is not particularly limited. The main characteristic of the polymer is MFR (Melt Flo
w Rate), softening point and the like. Of these, MFR
(JISK7210) is 0.2 to 50 g / 10 minutes, preferably 1.
It is 0-20g / 10 minutes. On the other hand, the melting point (DSC method) is generally in the range of 135 to 170 ° C., preferably 1
40-155 degreeC.
【０００７】本発明においては、上記熱可塑性エラスト
マーに他の重合体を混合することができる。例えばポリ
エチレン（ＬＤＰＥ，ＭＤＰＥ，ＨＤＰＥ，ＬＬＤＰ
Ｅ）、α−オレフィンと極性モノマーとの共重合体（Ｅ
ＶＡ，ＥＡ，ＥＥＡ）などを挙げることができる。In the present invention, the thermoplastic elastomer may be mixed with another polymer. For example, polyethylene (LDPE, MDPE, HDPE, LLDP
E), a copolymer of α-olefin and a polar monomer (E
VA, EA, EEA) and the like.
【０００８】本発明における熱可塑性エラストマーと他
の重合体の混合比は、特に限定するもではないが、熱可
塑性エラストマーが１０〜８０重量部で、他の重合体が
９０〜２０重量部である。以上の重合体を用いることに
より、本発明では導通抵抗が大きく変わる温度（スイッ
チング温度，Ｔｓ）が、組成物中の重合体の融点近傍で
認められる。The mixing ratio of the thermoplastic elastomer to the other polymer in the present invention is not particularly limited, but the thermoplastic elastomer is 10 to 80 parts by weight and the other polymer is 90 to 20 parts by weight. . By using the above polymer, the temperature (switching temperature, Ts) at which the conduction resistance greatly changes in the present invention is recognized near the melting point of the polymer in the composition.
【０００９】本発明における導電性材料は、ファーネス
ブラック、ケッチェンブラックなどのカーボンブラッ
ク、これらの極性モノマーによるグラフト物、金属メッ
キカーボンブラック、グラファイトなどを挙げることが
できるが、さらにニッケル、コバルト、銀、銅などの金
属やこれらに代表される金属の合金を用いることができ
る。以上の材料の形態は特に限定するものではないが、
一般的には粒状体が用いられ、例えばカーボンブラック
の場合には、１０〜１００nmの径の粒状物が用いられ
る。本発明における導電性材料の重合体に対する添加量
は導電性材料の種類にもよるが、一般的には２０〜１０
００重量部であり、好ましくは１００〜８００重量部で
ある。Examples of the conductive material in the present invention include carbon black such as furnace black and Ketjen black, graft products of these polar monomers, metal plated carbon black, graphite and the like, and further nickel, cobalt and silver. Metals such as copper and copper, and alloys of metals represented by these metals can be used. The form of the above materials is not particularly limited,
Generally, a granular material is used. For example, in the case of carbon black, a granular material having a diameter of 10 to 100 nm is used. The amount of the conductive material added to the polymer in the present invention depends on the type of the conductive material, but is generally 20 to 10.
The amount is 00 parts by weight, preferably 100 to 800 parts by weight.
【００１０】本発明においては、導電性材料の他に、他
の添加剤、例えば無機充填材、酸化防止剤、帯電防止
剤、シランカップリング剤等を添加することができる。In the present invention, in addition to the conductive material, other additives such as an inorganic filler, an antioxidant, an antistatic agent, a silane coupling agent and the like can be added.
【００１１】本発明における重合体、導電性材料等の組
成物の混合は、ロール、バンバリーミキサー、ヘンシェ
ルミキサー、ブラベンダープラストグラフ、押出機（単
軸、多軸）等の混練装置を用いて行うことができる。さ
らに本発明においては、通常、圧縮成形、押出成形、射
出成形等の成形法を用いて、プレート、シート、フィル
ム状の導電性複合体を作製することができる。Mixing of the composition such as the polymer and the conductive material in the present invention is carried out by using a kneading device such as a roll, a Banbury mixer, a Henschel mixer, a Brabender plastograph, an extruder (single-screw or multi-screw). be able to. Furthermore, in the present invention, a plate, sheet, or film-shaped conductive composite can be usually produced by using a molding method such as compression molding, extrusion molding, or injection molding.
【００１２】本発明における導電性複合体中の重合体
は、一般的には架橋されるが、ｔ−ブチルクミルパーオ
キサイド、２，５ジメチル−ジ（ｔ−ブチルパーオキ
シ）ヘキサン、２，５−ジメチル−ジ（ｔ−ブチルパー
オキシ）ヘキシン−３等を有機過酸化物を用いる化学架
橋法、ポリオレフィンにビニルシランをグラフトした
後、水分の存在下でシロキサン縮合反応による架橋を行
うシラン架橋法、さらには、電子線などを用いる放射線
架橋法のいずれの方法も用いることができる。The polymer in the conductive composite of the present invention is generally crosslinked, but t-butylcumyl peroxide, 2,5 dimethyl-di (t-butylperoxy) hexane, 2,5 -Chemical cross-linking method using dimethyl-di (t-butylperoxy) hexyne-3 or the like with an organic peroxide, silane cross-linking method in which vinyl silane is grafted onto polyolefin and then cross-linked by siloxane condensation reaction in the presence of water, Furthermore, any method of radiation crosslinking using an electron beam or the like can be used.
【００１３】本発明において、導電性複合体はニッケ
ル、銅等の電極材を熱圧着等の方法により接続される
が、さらに、成形歪の緩和、内部構造の安定化の目的の
ために熱処理を施すのが一般的である。なお、この熱処
理は導電性複合体と電極材の接続前、接続中または接続
後に行っても良い。In the present invention, the conductive composite is connected to an electrode material such as nickel or copper by a method such as thermocompression bonding. Further, heat treatment is performed for the purpose of relaxing molding strain and stabilizing the internal structure. It is generally applied. Note that this heat treatment may be performed before, during, or after the connection between the conductive composite and the electrode material.
【００１４】[0014]
【作用】本発明は、重合体と導電性材料からなる組成物
において、重合体がホモＰＰと、エチレンとプロピレン
のランダム共重合体が直接重合して得られる熱可塑性エ
ラストマーの少なくとも架橋物を主体とするために、こ
れを成形して得られる導電性複合体のＴｓは、ポリエチ
レン系樹脂の場合とほぼ同等で、温度と導通抵抗の関係
でヒステレシスが少なく再現性に優れた導電性複合体を
得ることができる。この理由としては推論の域を出ない
が、ホモＰＰ部分が一種の固定点の役割をすることによ
り、エチレン／プロピレン共重合体部の熱膨張に伴う導
電性材料間の間隔変化の再現性が良くなり、その結果、
従来のポリエチレン系樹脂マトリックスの場合とＴｓは
概ね同等でありながら、より再現性に優れた特性を示し
たものと考えられる。The present invention mainly comprises at least a crosslinked product of a thermoplastic elastomer obtained by directly polymerizing a homo-PP and a random copolymer of ethylene and propylene in a composition comprising a polymer and a conductive material. Therefore, the Ts of the conductive composite obtained by molding this is almost the same as that of the polyethylene resin, and a conductive composite having less hysteresis due to the relationship between temperature and conduction resistance and excellent in reproducibility is obtained. Obtainable. The reason for this is beyond speculation, but because the homo PP part plays a role of a kind of fixed point, the reproducibility of the spacing change between the conductive materials due to the thermal expansion of the ethylene / propylene copolymer part is improved. And as a result,
It is considered that the Ts was almost the same as that of the conventional polyethylene resin matrix, but exhibited a more excellent reproducibility.
【００１５】[0015]
実施例１ 表１に示す配合組成物を、８インチロールを用いて１６
０℃で１０分間混練後、１６０℃、５分間プレスし（１
５０kg/cm2）、厚み約０．８mmのシート（１０mm×１０
mm）を成形した。Example 1 The compounding composition shown in Table 1 was used for 16
After kneading at 0 ° C for 10 minutes, press at 160 ° C for 5 minutes (1
50kg / cm 2 ), 0.8mm thick sheet (10mm × 10)
mm) was molded.
【００１６】[0016]
【表１】 配 合 ──────────────────────────────── 材 料 添加量（重量部） ──────────────────────────────── 熱可塑性エラストマー （トクヤマ,P.E.R:MI;8,融点;143℃, 比重;0.88) 60 ポリエチレン （住友化学;MI;10, 融点;125℃, 比重;0.935) 40 導電性材料 (ファーネスフ゛ラック:平均粒径,50nm) 100 架橋助剤(トリメチロールフ゜ロハ゜ントリアクリレート) 1.0 酸化防止剤(Irganox1010) 0.5 ────────────────────────────────[Table 1] Allocation ──────────────────────────────── Material addition amount (parts by weight) ──── ──────────────────────────── Thermoplastic elastomer (TOKUYAMA, PER: MI; 8, melting point; 143 ℃, specific gravity; 0.88) 60 Polyethylene (Sumitomo Chemical; MI; 10, melting point; 125 ° C, specific gravity; 0.935) 40 Conductive material (furnace black: average particle size, 50 nm) 100 Cross-linking aid (trimethylol propane triacrylate) 1.0 Antioxidant (Irganox 1010) 0.5 ─────────────────────────────────
【００１７】該方法により得られた導電性複合体に５Mr
adの電子線照射を行った後、５mm×１０mmの大きさに切
り出し、両面に金属電極（ニッケル箔、厚み；３００n
m）を１６５℃で熱圧着し、該電極からリード線をはん
だ接続して取り出し温度と導通抵抗の関係を測定した。
また、降温後の復帰性を確認するために、室温での導通
抵抗を再測定した。結果を表２に示す。The conductive composite obtained by the method contains 5Mr
After irradiating the electron beam of ad, it is cut into a size of 5mm x 10mm, and metal electrodes (nickel foil, thickness; 300n) on both sides
m) was thermocompression bonded at 165 ° C., a lead wire was soldered from the electrode, and the relationship between the temperature and the conduction resistance was measured.
Further, the conduction resistance at room temperature was measured again in order to confirm the recoverability after cooling. Table 2 shows the results.
【００１８】[0018]
【表２】 導 通 抵 抗 測 定 結 果 ───────────────────────────────── 項 目 実施例１ 実施例２ 実施例３ 比較例 ───────────────────────────────── R25 0.040 0.030 0.035 0.050 R110 1.2M 1.1M 1.5M 1.2M R110/R25 3.0×10 3.7×10 4.3×10 2.4×10 R25 ＊ 0.042 0.034 0.037 0.10 Ts（℃) 130 131 129 120 ───────────────────────────────── Ｒ２５ ：２５℃での導通抵抗（Ω） Ｒ１１０：１１０℃での導通抵抗（Ω） Ｒ２５＊：２５℃に降温後での導通抵抗（Ω）[Table 2] General resistance measurement result ───────────────────────────────── Item Item Example 1 Example 2 Example 3 Comparative example ───────────────────────────────── R25 0.040 0.030 0.035 0.050 R110 1.2M 1.1 M 1.5M 1.2M R110 / R25 3.0 × 10 3.7 × 10 4.3 × 10 2.4 × 10 R25 * 0.042 0.034 0.037 0.10 Ts (℃) 130 131 129 120 ──────────────── ───────────────── R25: Conduction resistance at 25 ℃ (Ω) R110: Conduction resistance at 110 ℃ (Ω) R25 *: Conduction after cooling to 25 ℃ Resistance (Ω)
【００１９】実施例２ 導電性材料をニッケル粒子（約８〜１０ミクロン）と
し、７２０重量部加えた以外、実施例１と同様にして温
度−導通抵抗の関係を測定した。結果を表２に併記し
た。Example 2 The temperature-conduction resistance relationship was measured in the same manner as in Example 1 except that nickel particles (about 8 to 10 microns) were used as the conductive material and 720 parts by weight was added. The results are also shown in Table 2.
【００２０】実施例３ 導電性材料として、ポリスチレン粒子に金メッキをした
粒子（約１００nm）を用いた（３００重量部）以外、重
量部２と同様にして、温度−導通抵抗の関係を測定し
た。結果を表２に併記した。Example 3 The temperature-conduction resistance relationship was measured in the same manner as in the weight part 2 except that polystyrene particles were plated with gold (about 100 nm) (300 parts by weight) as the conductive material. The results are also shown in Table 2.
【００２１】比較例 表３に示す配合を用いて、実施例１と同様にして５mm×
１０mmの導電性複合体試料を作製し、温度と導通抵抗の
関係を測定した。結果を表２に併記した。Comparative Example 5 mm × in the same manner as in Example 1 except that the formulations shown in Table 3 were used.
A 10 mm conductive composite sample was prepared and the relationship between temperature and conduction resistance was measured. The results are also shown in Table 2.
【００２２】[0022]
【表３】 配 合 ─────────────────────────────────── 材 料 添加量（重量部） ─────────────────────────────────── ポリエチレン（住友化学;MI;10, 融点;125℃, 比重;0.935) 100 導電性材料 (ファーネスフ゛ラック:平均粒径,50nm) 100 酸化防止剤(Irganox1010) 0.5 ───────────────────────────────────[Table 3] Allocation ─────────────────────────────────── Material addition amount (parts by weight) ─ ────────────────────────────────── Polyethylene (Sumitomo Chemical; MI; 10, melting point; 125 ℃, specific gravity; 0.935) 100 Conductive material (furnace black: average particle size, 50 nm) 100 Antioxidant (Irganox1010) 0.5 ─────────────────────────── ─────────
【００２３】[0023]
【発明の効果】本発明によれば、ホモポリプロピレン
と、エチレンとプロピレンのランダム共重合体が直接重
合して得られる熱可塑性エラストマーの架橋物を含む組
成物を用いることにより、スイッチング温度はポリエチ
レンの例とほぼ同じで、導通抵抗の自己復帰性に優れる
特性を持った導電性複合体を得ることができる。EFFECTS OF THE INVENTION According to the present invention, by using a composition containing a homopolypropylene and a crosslinked product of a thermoplastic elastomer obtained by directly polymerizing a random copolymer of ethylene and propylene, the switching temperature of polyethylene is Almost the same as the example, it is possible to obtain a conductive composite having excellent characteristics of self-recovery of conduction resistance.
─────────────────────────────────────────────────────
─────────────────────────────────────────────────── ───
【手続補正書】[Procedure amendment]
【提出日】平成８年３月２７日[Submission date] March 27, 1996
【手続補正１】[Procedure Amendment 1]
【補正対象書類名】明細書[Document name to be amended] Statement
【補正対象項目名】００１８[Correction target item name] 0018
【補正方法】変更[Correction method] Change
【補正内容】[Correction content]
【００１８】[0018]
【表２】 導 通 抵 抗 測 定 結 果 ───────────────────────────────── 項 目 実施例１ 実施例２ 実施例３ 比較例 ───────────────────────────────── R25 0.040 0.030 0.035 0.050 R110 1.2M 1.1M 1.5M 1.2M R110/R25 3.0×107 3.7×107 4.3×107 2.4×107 R25 ＊ 0.042 0.034 0.037 0.10 Ts（℃) 130 131 129 120 ───────────────────────────────── Ｒ２５ ：２５℃での導通抵抗（Ω） Ｒ１１０：１１０℃での導通抵抗（Ω） Ｒ２５＊：２５℃に降温後での導通抵抗（Ω）[Table 2] General resistance measurement results ───────────────────────────────── Item Item Example 1 Example 2 Example 3 Comparative example ───────────────────────────────── R25 0.040 0.030 0.035 0.050 R110 1.2M 1.1 M 1.5M 1.2M R110 / R25 3.0 × 10 7 3.7 × 10 7 4.3 × 10 7 2.4 × 10 7 R25 * 0.042 0.034 0.037 0.10 Ts (℃) 130 131 129 120 ───────────── ───────────────────── R25: Conductive resistance at 25 ° C (Ω) R110: Conductive resistance at 110 ° C (Ω) R25 *: Temperature drop to 25 ° C Lateral conduction resistance (Ω)
Claims (3)
体とホモポリプロピレンとが直接重合して得られる熱可
塑性エラストマーを含む重合体と、導電性材料からなる
導電性複合材料組成物において、前記重合体１００重量
部に対して導電性材料が２０〜１０００重量部含まれる
こと特徴とする導電性複合材料組成物。1. A conductive composite material composition comprising a conductive elastomer and a polymer containing a thermoplastic elastomer obtained by directly polymerizing a random copolymer of ethylene and propylene and homopolypropylene, wherein the polymer 100 is used. A conductive composite material composition, wherein the conductive material is contained in an amount of 20 to 1000 parts by weight with respect to parts by weight.
成形してなる導電性複合体。2. A conductive composite body obtained by molding the conductive composite material composition according to claim 1.
イッチング温度（Ｔｓ）を有することを特徴とする請求
項２記載の導電性複合体。3. The conductive composite body according to claim 2, wherein the conductive composite body has at least one switching temperature (Ts).
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP12202795A JPH08316005A (en) | 1995-05-22 | 1995-05-22 | Conductive composite material composition and conductive complex obtained by molding such composition |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP12202795A JPH08316005A (en) | 1995-05-22 | 1995-05-22 | Conductive composite material composition and conductive complex obtained by molding such composition |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH08316005A true JPH08316005A (en) | 1996-11-29 |
Family
ID=14825786
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP12202795A Pending JPH08316005A (en) | 1995-05-22 | 1995-05-22 | Conductive composite material composition and conductive complex obtained by molding such composition |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH08316005A (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6607679B2 (en) | 2001-01-12 | 2003-08-19 | Tdk Corporation | Organic PTC thermistor |
-
1995
- 1995-05-22 JP JP12202795A patent/JPH08316005A/en active Pending
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6607679B2 (en) | 2001-01-12 | 2003-08-19 | Tdk Corporation | Organic PTC thermistor |
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