JP3669180B2 - Conductive composition for improving connection resistance value - Google Patents
Conductive composition for improving connection resistance value Download PDFInfo
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- JP3669180B2 JP3669180B2 JP30065898A JP30065898A JP3669180B2 JP 3669180 B2 JP3669180 B2 JP 3669180B2 JP 30065898 A JP30065898 A JP 30065898A JP 30065898 A JP30065898 A JP 30065898A JP 3669180 B2 JP3669180 B2 JP 3669180B2
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- connection resistance
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Description
【０００１】
【産業上の利用分野】
本発明は新規な導電性組成物に関し、従来接続抵抗値が高くなってしまう電極金属であるアルミニウム、クロム等に対しても低く、安定した接続抵抗値が得られる導電性組成物を提供するものである。
【０００２】
【従来の技術】
従来から導電性樹脂組成物に使用されている導電フィラーは銀粉が一般的である。しかし、導電フィラーとして銀粉のみを含有する導電性組成物はアルミ電極との接続抵抗値が高くなる。（特開昭６２−９０９３８）また発明者の実験によればクロムもしくはクロムを含有するステンレスに対しても接続抵抗値が高くなることがわかっている。
【０００３】
【発明が解決しようとする課題】
電極ａと電極ｂを導電性組成物で接続したした場合の電極間接続抵抗値は、下式であらわすことができる。
【０００４】
Ｒｔｏ＝Ｒａ ＋Ｒｂ ＋α （式１）
【０００５】
ここで、Ｒｔｏは実際の電極間の接続抵抗の測定値、Ｒａ およびＲｂ は電極ａと導電性組成物との接続抵抗値および電極ｂと導電性組成物との接続抵抗値でありαは電極間の導電性組成物そのものの抵抗値である。
【０００６】
つまり、導電性組成物の抵抗値αが低くても、電極ａ、ｂの材質と導電性組成物の相性によっては界面での接続抵抗値Ｒａ、Ｒｂが高くなり、電極間接続抵抗値Ｒｔｏが高くなる。
【０００７】
しかし、導電性組成物が電極間の接続材として使用される場合、特に高周波で低電流の接続の場合は、電極間接続抵抗値を低く安定化させることが強く要求される。
【０００８】
接続抵抗値の高い導電性組成物で接続した場合の課題としては、例えばアナログ回路で使用された場合、電極の接続部分で電圧降下を起こしデバイスが誤動作するか場合によっては動作しない恐れもある。また水晶振動子の電極の接続材に接続抵抗値の高い導電性樹脂材料が使用された場合、クリスタルインピーダンス（ＣＩ値）が高くなり周波数変動の原因となる。
【０００９】
このようなアルミ電極を導電性組成物で接続するとその接続抵抗値に高くなる現象に対して、特開平６−３３３９８３ではアルミ電極の酸化被膜をニッケル粒子で破り銀粉を圧入して接続抵抗値を下げる技術を開示している。
【００１０】
【課題を解決するための手段】
本発明は、バインダーと導電フィラーで構成される導電性組成物において、バインダーと導電フィラーで構成される導電性組成物において、前記導電フィラーが、平均粒径の中心値を２０μｍ以下とする銀粉と、当該銀粉よりも小径の平均粒径を有するニッケル粉とを含有するとともに、前記銀粉とニッケル粉の配合比が、重量比で前者６０〜４０に対し後者４０〜６０とする電極間を電気的に接続するための低接続抵抗の導電性接着組成物を用いることにより、アルミ、クロムまたはステンレスとの接続抵抗値を低くすることができる。
【００１１】
上記バインダーは既存の有機バインダー、無機バインダーのいずれでもよいが、好ましくはエポキシ樹脂、ウレタン樹脂、シリコーン樹脂、アクリル樹脂、またはポリイミド樹脂の熱硬化性樹脂のうちから一種類以上を選ぶことができる。
【００１２】
また、上記導電フィラーの形状としては鱗片状（フレーク状）、粒状（球形が好ましい）、薄片状、樹枝状、不規則形のいずれを使用しても良いが、導電性組成物そのものの抵抗値（体積固有抵抗値）を低くさせるためと、塗布性を良くするためには、鱗片状と粒状を組み合わせて使用するのが好ましい。特に銀粉は鱗片状を使用するのが好ましい。ニッケル粉は、銀粉より小さい平均粒径の粒状が好ましい。
【００１３】
さらに、銀粉の平均粒径の中心値が２０μｍ以下であるが好ましく、鱗片状でその中心値が１５μｍ以下が特に好ましい。さらに、ニッケル粉は平均粒径の中心値は５μｍ以下が好ましく、特に球状で中心値が３μｍが好ましい。
【００１４】
本発明の好ましい導電性組成物の例として、バインダーが熱硬化性樹脂１０〜３０重量部に対して、平均粒径の中心値が１０μｍの鱗片状銀粉が８２重量部〜１０重量部、平均粒径の中心値が３μｍの粒状ニッケル粉が３〜７５重量部（銀粉／ニッケル粉の重量比＝８２／３〜１０／７５）で構成される組成物である。
【００１５】
さらに導電性組成物の好ましい例として、熱硬化性樹脂がフェノール硬化剤を含むエポキシ樹脂、または付加型シリコーン樹脂１５〜２０重量部に対して、平均粒径の中心値が１０μｍの鱗片状銀粉が６０〜４０重量部、平均粒径の中心値が３μｍの粒状ニッケル粉がの重量比が４０〜６０重量部（銀粉／ニッケル粉の重量比＝６０／４０〜４０／６０）で、導電フィラーとしての銀粉とニッケル粉の合計が８０〜８５重量部で構成される組成物である。
【００１６】
前記において銀粉の割合が多いと導電性組成物としての体積固有抵抗値は低くなるが接続抵抗値は低くならない。逆にニッケル粉の割合が多いと接続抵抗値は銀粉単体の組成物と比べれば低くなるが導電性組成物としての体積固有抵抗値が高くなってしまい前述（式１）のαが高くなり接続抵抗値は低くならない。
【００１７】
本発明において、導電フィラーの分散性を改良するための界面活性剤、酸化による接続抵抗値および体積固有抵抗値上昇を防ぐための酸化防止剤、樹脂の劣化防止剤、粘度調整のための溶剤またはチクソトロピック剤、接着性を改良するための粘着剤またはカップリング剤などの既知の改質剤を添加してもよい。
【００１８】
【作用】
本発明の導電性組成物の接続抵抗値が、従来の導電性組成物に比べて低くなる理由は定かではない。
【００１９】
しかし、前述のＲｔｏ＝Ｒａ ＋Ｒｂ ＋α （式１）の電極ａと導電性組成物との接続抵抗値Ｒａおよび電極ｂと導電性組成物との接続抵抗値Ｒｂは導電性組成物に含有される導電フィラーとの電気的相性があると考えられる。これは特開昭５９−１２４７０６にも記述されているように銀−パラジウム電極を形成することでハンダ食われ現象を防止するというのがあるが、これはハンダの拡散を防止している。すなわち電極と導電性組成物の界面での電気的相性は、電極材と導電フィラーの拡散現象（合金化）が関係しており電極材と導電フィラーの組み合わせにおいて合金化しやすい組み合わせになると界面での接続抵抗値が高くなり、合金化しにくい組み合わせなら接続抵抗値が低くなると推定する。従来、銀ペーストでは接続抵抗値が高かった電極材に対してニッケル粉が界面での接続抵抗値を低減させ、導電性組成物としての抵抗（体積固有抵抗値）は銀粉によるものと推定する。
【００２０】
また、前述の先行技術として掲げた特開平６−３３３９８３もアルミ電極の接続における接続抵抗値の低減するが、導電性接着剤の成分であるニッケル粒子でアルミ電極の酸化被膜を破る作用により、接続抵抗値の低下を達成している。このため、ＩＣチップと回路基板上のアルミ電極を当該導電性接着剤を挟んで接続する際に前記酸化被膜を破る程の加圧が必要となる。
【００２１】
しかし、本発明では大きい平均粒径の銀粉とそれより小さい平均粒径のニッケル粉との組み合わせからなりので、接続の際に前記のような加圧することなしに低い接続抵抗値が得られる。つまり、合金化しにくく平均粒径の小さいニッケル粉が銀粉を覆うように存在するので、銀の合金化による接続抵抗値の上昇を回避するからである。
【００２２】
【発明の実施の形態】
実施例１及び参考例１〜２
バインダーとして軟質エポキシ樹脂（Ｒ-１５２、三井石油化学社製）１００重量部に対して、フェノール樹脂（ＰＳＭ-４２６１、群栄化学工業社製）２０重量部イミダゾール（２ＰＨＺ、四国化成社製）３重量部を混合して熱硬化性の軟質エポキシ樹脂組成物を製造した。この組成物１５重量部に有機溶剤を１０重量部を混合した。さらにこのバインダーに中心粒径１０μｍの鱗片状銀粉と中心粒径３μｍの粒状ニッケル粉を混合比率を変えて混練し３種類の導電性樹脂組成物を製造した。なお、比較例１として前述のバインダーに中心粒径１０μｍの鱗片状銀粉のみを混練した導電性樹脂組成物を製造した。実施例１、参考例１〜２、及び比較例１の組成物の配合を表１にしめす。
【００２３】
実施例２及び参考例３〜４
バインダーとして硬質エポキシ樹脂（エピコート８０７、油化シェルエポキシ社製）１００重量部に対して、フェノール樹脂（ＰＳＭ-４２６１、群栄化学工業社製）２０重量部イミダゾール（２ＰＨＺ、四国化成社製）３重量部を混合して熱硬化性の硬質エポキシ樹脂組成物を製造した。実施例１、参考例１〜２と同じように中心粒径１０μｍの鱗片状銀粉と中心粒径３μｍの粒状ニッケル粉を混合比率を変えて混練し３種類の導電性樹脂組成物を製造した。なお、比較例２として同様に中心粒径１０μｍの鱗片状銀粉のみを混練した導電性樹脂組成物を製造した。実施例２、参考例３〜４、及び比較例２の組成物の配合を表２にしめす。
【００２４】
実施例３及び参考例５〜６
バインダーとして付加型加熱硬化シリコーン樹脂（ＴＳＥ−３２１２、東芝シリコーン社製）１５重量部に有機溶剤を１０重量部を混合した。さらにこのバインダーに中心粒径１０μｍの鱗片状銀粉と中心粒径３μｍの粒状ニッケル粉を混合比率を変えて混練し３種類の導電性樹脂組成物を製造した。なお、比較例３として同様に中心粒径１０μｍの鱗片状銀粉のみを混練した導電性樹脂組成物を製造した。実施例３、参考例５〜６、及び比較例３の組成物の配合を表３にしめす。
【００２５】
実施例および比較例の導電性樹脂組成物を、種々の基板に塗布し適当なギャップで銅線と接着させ基板と銅線との抵抗値を測定し、その結果を各配合に対応して表１〜３に示す。
【００２６】
【表１】
【表２】
【表３】
【発明の効果】
本発明の導電性組成物は、接続抵抗値が低く且つ安定しているため接続抵抗値が低いことを要求されるチップ部品の導電接続に用いることができる。特に従来の導電性樹脂組成物では接続抵抗値が高くなってしまう相手電極材に対しても低い接続抵抗値が得られるため、例えばアナログ回路のデバイスの接続材で使用されても、電極の接続部分で電圧降下が少なくデバイスが誤動作する心配がない。また水晶振動子の電極の接続材に使用されてもクリスタルインピーダンスが低くなるため周波数変動の少ない水晶振動子が得られる。
【００３０】
本発明は従来技術では接続抵抗値が高くなってしまう電極材、例えばアルミ、クロムまたはクロムを含むステンレス等に対しても低く安定した接続抵抗値を得られる導電性組成物を提供することにより上記のような問題点を解決するものである。[0001]
[Industrial application fields]
The present invention relates to a novel conductive composition, and provides a conductive composition that can provide a stable connection resistance value, which is low compared to conventional electrode metals such as aluminum and chromium, which have increased connection resistance values. It is.
[0002]
[Prior art]
Conventionally, silver powder is generally used as the conductive filler used in the conductive resin composition. However, the conductive composition containing only silver powder as the conductive filler has a high connection resistance value with the aluminum electrode. Further, according to the experiment by the inventors, it has been found that the connection resistance value is increased even for chromium or stainless steel containing chromium.
[0003]
[Problems to be solved by the invention]
The interelectrode connection resistance value when the electrode a and the electrode b are connected by the conductive composition can be expressed by the following equation.
[0004]
R to = R a + R b + α (Formula 1)
[0005]
Here, R to is a measured value of connection resistance between actual electrodes, R a and R b are connection resistance values between the electrode a and the conductive composition, and connection resistance values between the electrode b and the conductive composition. α is the resistance value of the conductive composition itself between the electrodes.
[0006]
That is, even if the resistance value α of the conductive composition is low, the connection resistance values R a and R b at the interface are high depending on the compatibility of the material of the electrodes a and b and the conductive composition, and the interelectrode connection resistance value is high. R to increases.
[0007]
However, when the conductive composition is used as a connection material between the electrodes, particularly in the case of connection at a high frequency and a low current, it is strongly required to stabilize the interelectrode connection resistance value low.
[0008]
As a problem when connecting with a conductive composition having a high connection resistance value, for example, when used in an analog circuit, there is a possibility that a voltage drop occurs at the connection portion of the electrode and the device malfunctions or does not operate depending on the case. Further, when a conductive resin material having a high connection resistance value is used as the connection material for the electrodes of the crystal resonator, the crystal impedance (CI value) is increased, which causes frequency fluctuation.
[0009]
When such an aluminum electrode is connected with a conductive composition, the connection resistance value is increased. In Japanese Patent Laid-Open No. 6-333983, the oxide film of the aluminum electrode is broken with nickel particles and silver powder is press-fitted to reduce the connection resistance value. The technology to lower is disclosed.
[0010]
[Means for Solving the Problems]
The present invention provides a conductive composition comprising a binder and a conductive filler, wherein the conductive filler comprises a silver powder having a mean value of an average particle diameter of 20 μm or less. In addition, the nickel powder having an average particle diameter smaller than that of the silver powder is contained, and the mixture ratio of the silver powder and the nickel powder is electrically between the electrodes 40-60 with respect to the former 60-40 by weight ratio. By using a conductive adhesive composition having a low connection resistance for connection to aluminum, the connection resistance value with aluminum, chromium or stainless steel can be lowered.
[0011]
The binder may be an existing organic binder or inorganic binder, but preferably one or more of thermosetting resins such as epoxy resin, urethane resin, silicone resin, acrylic resin, or polyimide resin can be selected.
[0012]
Moreover, as the shape of the conductive filler, any of scaly (flakes), granular (preferably spherical), flaky, dendritic, and irregular shapes may be used, but the resistance value of the conductive composition itself. In order to reduce the (volume specific resistance value) and to improve the coating property, it is preferable to use a combination of scaly and granular. In particular, it is preferable to use a scaly silver powder. The nickel powder is preferably granular with an average particle size smaller than silver powder.
[0013]
Further, the central value of the average particle diameter of the silver powder is preferably 20 μm or less, and is preferably scaly and has a central value of 15 μm or less. Furthermore, the nickel powder preferably has a center value of the average particle diameter of 5 μm or less, particularly spherical and preferably has a center value of 3 μm.
[0014]
As an example of a preferable electroconductive composition of the present invention, a binder is 10 to 30 parts by weight of a thermosetting resin, a scaly silver powder having a mean particle diameter of 10 μm is 82 parts by weight to 10 parts by weight, and an average particle This is a composition comprising 3 to 75 parts by weight of granular nickel powder having a median diameter of 3 μm (silver powder / nickel powder weight ratio = 82/3 to 10/75).
[0015]
Furthermore, as a preferable example of the conductive composition, a scale-like silver powder having a median average particle diameter of 10 μm is used with respect to 15 to 20 parts by weight of an epoxy resin whose thermosetting resin contains a phenol curing agent or an addition-type silicone resin. As a conductive filler, the weight ratio of granular nickel powder having an average particle diameter of 3 μm is 40 to 60 parts by weight (silver powder / nickel powder weight ratio = 60/40 to 40/60). The total of silver powder and nickel powder is composed of 80 to 85 parts by weight.
[0016]
In the above, when the proportion of silver powder is large, the volume resistivity value as the conductive composition is lowered, but the connection resistance value is not lowered. On the contrary, when the proportion of nickel powder is large, the connection resistance value is lower than that of the composition of the silver powder alone, but the volume resistivity value as the conductive composition is increased and α in the above (Equation 1) is increased and the connection is increased. Resistance value does not become low.
[0017]
In the present invention, a surfactant for improving the dispersibility of the conductive filler, an antioxidant for preventing an increase in connection resistance value and volume specific resistance value due to oxidation, a resin deterioration preventing agent, a solvent for adjusting viscosity, or You may add known modifiers, such as a thixotropic agent, the adhesive for improving adhesiveness, or a coupling agent.
[0018]
[Action]
The reason why the connection resistance value of the conductive composition of the present invention is lower than that of the conventional conductive composition is not clear.
[0019]
However, the connection resistance value R b of the aforementioned R to = R a + R b + α connection resistance R a and the electrode b and the conductive composition of the electrode a and the conductive composition (Formula 1) is electrically conductive composition It is considered that there is an electrical compatibility with the conductive filler contained in the product. As described in JP-A-59-124706, a silver-palladium electrode is formed to prevent a solder erosion phenomenon, which prevents the diffusion of solder. In other words, the electrical compatibility at the interface between the electrode and the conductive composition is related to the diffusion phenomenon (alloying) between the electrode material and the conductive filler. It is presumed that the connection resistance value becomes low if the connection resistance value becomes high and it is difficult to alloy. Conventionally, nickel powder reduces the connection resistance value at the interface with respect to an electrode material having a high connection resistance value in silver paste, and the resistance (volume specific resistance value) as a conductive composition is estimated to be due to silver powder.
[0020]
Japanese Patent Laid-Open No. 6-333983 listed as the above prior art also reduces the connection resistance value in the connection of aluminum electrodes, but the connection by the action of breaking the oxide film of the aluminum electrode with nickel particles that are components of the conductive adhesive. The resistance value has been lowered. For this reason, when connecting an IC chip and the aluminum electrode on a circuit board on both sides of the said conductive adhesive, the pressurization which breaks the said oxide film is needed.
[0021]
However, in the present invention, since it consists of a combination of silver powder having a large average particle diameter and nickel powder having a smaller average particle diameter, a low connection resistance value can be obtained without pressurizing as described above. That is, since nickel powder which is difficult to alloy and has a small average particle diameter exists so as to cover the silver powder, an increase in connection resistance value due to silver alloying is avoided.
[0022]
DETAILED DESCRIPTION OF THE INVENTION
Example 1 and Reference Examples 1-2
As a binder, 100 parts by weight of a soft epoxy resin (R-152, manufactured by Mitsui Petrochemical Co., Ltd.), 20 parts by weight of a phenol resin (PSM-4261, manufactured by Gunei Chemical Industry Co., Ltd.), imidazole (2PHZ, manufactured by Shikoku Kasei Co., Ltd.) 3 A thermosetting soft epoxy resin composition was produced by mixing parts by weight. 10 parts by weight of an organic solvent was mixed with 15 parts by weight of this composition. Further, this binder was kneaded with flaky silver powder having a central particle diameter of 10 μm and granular nickel powder having a central particle diameter of 3 μm at different mixing ratios to produce three types of conductive resin compositions. As Comparative Example 1, a conductive resin composition was produced by kneading only the scaly silver powder having a center particle size of 10 μm with the above-mentioned binder. Table 1 shows the composition of the compositions of Example 1, Reference Examples 1 and 2, and Comparative Example 1.
[0023]
Example 2 and Reference Examples 3-4
As a binder, 100 parts by weight of hard epoxy resin (Epicoat 807, manufactured by Yuka Shell Epoxy Co., Ltd.), 20 parts by weight of phenol resin (PSM-4261, manufactured by Gunei Chemical Industry Co., Ltd.), imidazole (2PHZ, manufactured by Shikoku Kasei Co., Ltd.) 3 A thermosetting hard epoxy resin composition was produced by mixing parts by weight. In the same manner as in Example 1 and Reference Examples 1 and 2 , scaly silver powder having a central particle size of 10 μm and granular nickel powder having a central particle size of 3 μm were kneaded at different mixing ratios to produce three types of conductive resin compositions. In addition, the conductive resin composition which knead | mixed only the scaly silver powder with a center particle diameter of 10 micrometers similarly as the comparative example 2 was manufactured. Table 2 shows the composition of the compositions of Example 2, Reference Examples 3 to 4, and Comparative Example 2.
[0024]
Example 3 and Reference Examples 5-6
As a binder, 10 parts by weight of an organic solvent was mixed with 15 parts by weight of an addition-type thermosetting silicone resin (TSE-3212, manufactured by Toshiba Silicone). Further, this binder was kneaded with flaky silver powder having a central particle diameter of 10 μm and granular nickel powder having a central particle diameter of 3 μm at different mixing ratios to produce three types of conductive resin compositions. In addition, the conductive resin composition which knead | mixed only the scaly silver powder with a center particle diameter of 10 micrometers similarly as the comparative example 3 was manufactured. Table 3 shows the compositions of the compositions of Example 3, Reference Examples 5 to 6, and Comparative Example 3.
[0025]
The conductive resin compositions of Examples and Comparative Examples were applied to various substrates, adhered to copper wires with appropriate gaps, measured for resistance values between the substrates and the copper wires, and the results were shown corresponding to each formulation. 1-3.
[0026]
[Table 1]
[Table 2]
[Table 3]
【The invention's effect】
The conductive composition of the present invention has a low connection resistance value and is stable, and thus can be used for conductive connection of chip components that are required to have a low connection resistance value. In particular, since the conventional conductive resin composition can provide a low connection resistance value even with respect to the mating electrode material that results in a high connection resistance value, for example, even when used as a connection material for analog circuit devices, the electrode connection There is little voltage drop in the part, and there is no worry of device malfunction. Even if it is used as a connecting material for electrodes of a crystal resonator, the crystal impedance is low, so that a crystal resonator with little frequency fluctuation can be obtained.
[0030]
The present invention provides a conductive composition capable of obtaining a low and stable connection resistance value even with respect to electrode materials that have a high connection resistance value in the prior art, such as aluminum, chromium, or stainless steel containing chromium. It solves the following problems.
Claims (5)
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP30065898A JP3669180B2 (en) | 1998-10-22 | 1998-10-22 | Conductive composition for improving connection resistance value |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP30065898A JP3669180B2 (en) | 1998-10-22 | 1998-10-22 | Conductive composition for improving connection resistance value |
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| Publication Number | Publication Date |
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| JP2000133043A JP2000133043A (en) | 2000-05-12 |
| JP3669180B2 true JP3669180B2 (en) | 2005-07-06 |
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| JP30065898A Expired - Lifetime JP3669180B2 (en) | 1998-10-22 | 1998-10-22 | Conductive composition for improving connection resistance value |
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Families Citing this family (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6524721B2 (en) | 2000-08-31 | 2003-02-25 | Matsushita Electric Industrial Co., Ltd. | Conductive adhesive and packaging structure using the same |
| US8044330B2 (en) * | 2008-01-17 | 2011-10-25 | E.I. Du Pont De Nemours And Company | Electrically conductive adhesive |
| JP5417861B2 (en) * | 2009-01-23 | 2014-02-19 | 日亜化学工業株式会社 | Conductive material, manufacturing method thereof, electronic device including conductive material, light emitting device |
| CN108779373A (en) * | 2015-10-15 | 2018-11-09 | 汉高知识产权控股有限责任公司 | Nickel and contain purposes of the alloy of nickel as conductive filler in adhesive formulation |
| JP6309041B2 (en) * | 2016-05-09 | 2018-04-11 | サン電子工業株式会社 | Solid electrolytic capacitor |
| US10982120B2 (en) | 2016-09-06 | 2021-04-20 | Threebond Co., Ltd. | Thermocurable electroconductive adhesive |
| WO2021220976A1 (en) * | 2020-05-01 | 2021-11-04 | 昭栄化学工業株式会社 | Electroconductive resin composition and manufacturing method for electronic component |
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1998
- 1998-10-22 JP JP30065898A patent/JP3669180B2/en not_active Expired - Lifetime
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