JP2018109073A - Composite material composition, and paste agent using the same - Google Patents

Abstract

PROBLEM TO BE SOLVED: To improve adhesiveness and adhesion of a composite material to a base material such as copper, silver, aluminum, silicon and ferrite by combining low-melting glass used for sealing, adhesion and formation of a conductive joint portion with a resin material.SOLUTION: A composite material composition contains a low-melting glass component, and a resin component having no hydroxyl group and amino group, where the low-melting glass component contains VO, TeOand AgO, the total content of the VO, the TeOand the AgO in the low-melting glass component is 78 mol% or more, the contents of the TeOand the AgO are 1-2 times in a molar ratio with respect to the content of VO, and 0 or more and 20 mol% or less of one or more selected from BaO, WOand POis contained in the low-melting glass component as a first additional component, and 0.1 mol% or more and 2.0 mol% or less of one or more selected from YO, LaO, AlOand FeOis contained in the low-melting glass component as a second additional component.SELECTED DRAWING: None

Description

  The present invention relates to a composite material composition and a paste agent using the same.

  The resin material is characterized by being lightweight and easy to mold at a relatively low temperature as compared with other materials such as inorganic and metal. The application range of the resin material is very wide, and it is applied to semiconductor encapsulants and molding materials for various electric devices. Such resin materials are required to have improved adhesion to different materials such as inorganic and metal, heat dissipation, and thermal conductivity. Conventionally, the adhesion, heat dissipation, thermal conductivity, etc. of resin materials have been improved by the molecular design of resin materials and the addition of fillers, etc., but generally there is a trade-off between improving adhesiveness and improving heat dissipation and thermal conductivity. There was a problem of being in an off relationship.

  In addition, resin materials are used as insulating materials because of their high electrical resistance, but conversely, application to fields unprecedented can be considered by reducing their electrical resistance. Furthermore, although the resin material has a low gas barrier property, it can be considered that the gas barrier property is improved by combining with a glass.

  In Patent Document 1, in a composite material including a resin or rubber and oxide glass, the resin or rubber is dispersed in the oxide glass, or the oxide glass is dispersed in the resin or rubber. A composite material is disclosed in which the oxide glass softens and flows below the thermal decomposition temperature of the resin or rubber by heating. In Patent Document 1, in order to solve the low interfacial strength between the resin material and glass, which was a problem with the conventional glass fiber reinforced plastic, the interfacial strength is improved by using low-melting glass, and the resin material and glass are used. The mechanical strength of the composite material is improved. However, Patent Document 1 does not describe the detailed composition of the resin material and the low-melting glass for maximizing the effect and the phenomenon at the interface.

  In many electrical and electronic parts such as solar cells, image display devices, multilayer capacitors, crystal resonators, LEDs (light emitting diodes), and multilayer circuit boards, electrodes are formed by a conductive composition containing low-melting glass and metal particles. And wiring are formed. This composition is also used as a bonding material for conducting. Such a conductive composition is often applied in the form of a conductive glass paste similar to a glass frit for a low-temperature encapsulant, and this conductive glass paste is coated with copper by a screen printing method or a dispenser method. It is applied to a base material such as aluminum, ferrite, etc., dried and baked to form electrodes, wiring, conductive joints, and the like. During the formation, the low melting point glass contained in the conductive composition and the conductive glass paste using the conductive composition is softened and fluidized to sinter the metal particles or to adhere the composition to the substrate. I am letting. Therefore, such a composition is required to have high adhesion to the substrate and high adhesion.

JP2013-133342A

  As described above, in the development of resin materials, there has been a trade-off relationship between the improvement in adhesiveness and the improvement in heat dissipation and thermal conductivity. In addition, the resin material has a problem that the electric resistance is large and the gas barrier property is low. Then, this invention aims at solving the subject of these resin materials by compounding low melting glass and resin material.

  In addition, by combining low melting point glass used for sealing, adhesion, and formation of conductive joints with resin materials, composite materials for substrates such as copper, silver, aluminum, silicon, and ferrite It aims at improving adhesiveness and adhesiveness.

As a result of diligent research by the present inventors, it was found that the above problems can be solved by combining a low-polarity resin component and a low-melting glass component having a reduced crystallization tendency, thereby completing the invention. did. That is, the composite material composition of the present invention is a composite material composition comprising a low-melting glass component and a resin component having no hydroxyl group and amino group, wherein the low-melting glass component is V ₂ O ₅ , TeO ₂ and Ag ₂ O, the total content of V ₂ O ₅ , TeO ₂ and Ag ₂ O in the low melting point glass component is 78 mol% or more, and the content of TeO ₂ and Ag ₂ O is It is characterized by being 1 to 2 times in terms of molar ratio with respect to the content of V ₂ O ₅ .

  By compounding a resin component having a low polarity and a low melting point glass component, it is possible to obtain a composite composition having improved adhesion to a substrate and low electrical resistance. This composite material composition can be used as a paste agent or the like. Problems, configurations, and effects other than those described above will be clarified by the following description of the embodiments.

It is a figure for demonstrating the characteristic temperature of a low melting glass component. It is the figure which represented typically the cross section of the composite material composition which concerns on this invention. It is a figure for demonstrating the evaluation method of the adhesiveness in an Example.

Hereinafter, the present invention will be described in detail based on embodiments.
The composite material composition of the present invention comprises a low melting glass component and a resin component having no hydroxyl group and amino group.

The low melting point glass component includes V ₂ O ₅ , TeO ₂ and Ag ₂ O. The total content of V ₂ O ₅ , TeO ₂ and Ag ₂ O in the low-melting glass component is 78 mol% or more, and the content of TeO ₂ and Ag ₂ O is relative to the content of V ₂ O ₅ , respectively. The molar ratio is 1 to 2 times. Further, as the first additional component, one or more selected from BaO, WO ₃ and P ₂ O ₅ are contained in the low melting point glass component in an amount of 0 to 20 mol%, and the second additional component is Y ₂ O ₃ , La ₂ O. ₃ , Al ₂ O ₃ and Fe ₂ O ₃ are preferably contained in an amount of 0.1 mol% or more and 2.0 mol% or less in the low melting point glass component.

  The functions of vanadium oxide, tellurium oxide and silver oxide, which are the main components in the low melting point glass component, will be described below. Silver oxide is contained for lowering the characteristic temperature such as transition point, yield point, softening point, and improving chemical stability. Vanadium oxide is contained so that silver oxide is not reduced and metallic silver is not precipitated during preparation of the low-melting glass component. If silver oxide is not present in the low melting point glass component in the form of silver ions, the effect of lowering the characteristic temperature cannot be obtained. By increasing the content of silver oxide, that is, by increasing the amount of silver ions in the low-melting-point glass component, the characteristic temperature can be lowered, but in this case, precipitation of metallic silver is prevented. Or in order to suppress, it is also necessary to increase the content of vanadium oxide. When preparing the low melting point glass component, up to two monovalent silver ions can be contained for one pentavalent vanadium ion. Tellurium oxide is a vitrification component for vitrifying a low-melting glass component. If tellurium oxide is not contained, glass cannot be formed. However, up to one tetravalent tellurium ion is effective for one pentavalent vanadium ion, and if it exceeds this, a compound of tellurium and silver may be precipitated.

In consideration of the action of vanadium oxide, tellurium oxide and silver oxide as described above, the compound serving as the base of the low melting point glass component has a total content of V ₂ O ₅ , TeO ₂ and Ag ₂ O of 78 mol%. The content of TeO ₂ and Ag ₂ O is 1 to 2 times as the molar ratio with respect to the content of V ₂ O ₅ . When the composition is out of the range, metallic silver is precipitated during the preparation of the low melting point glass component, the effect of lowering the characteristic temperature is reduced, the crystal is markedly crystallized during the heating and baking, or the chemical stability is reduced. There is a possibility that problems such as lowering may occur.

Further, in order to easily obtain the low melting point glass component as a uniform glass state (amorphous state) and to reduce the crystallization tendency of the obtained low melting point glass component, BaO, It is effective to include one or more selected from WO ₃ and P ₂ O ₅ in the low melting point glass component in an amount of 0 to 20 mol%. If it exceeds 20 mol%, the melting point may increase.

Y ₂ O ₃ , La ₂ O ₃ , Al ₂ O _3, and Fe ₂ O ₃ contained as the second additional component have the effect of significantly reducing the crystallization tendency when contained in a small amount. In total, it is effective to adjust the content to 0.1 mol% or more and 2.0 mol or less in the low melting point glass component. If it exceeds 2.0 mol%, the characteristic temperature of the low-melting-point glass component such as transition point, yield point, softening point, etc. may increase, or conversely, the tendency to crystallize may increase.

  Moreover, it is preferable that the low melting glass component in this invention is a lead-free low melting glass component. Here, “lead-free” is to permit the inclusion of prohibited substances in the RoHS Directive (enforced July 1, 2006) within the specified value range. In the case of lead (Pb), it is 1000 ppm or less.

  In addition, the low melting point glass component contained in the composite material composition of the present invention preferably has a softening point of 280 ° C. or less, which is the second endothermic peak temperature by differential thermal analysis (DTA), and is further crystallized by DTA. The starting temperature is preferably 60 ° C. or more higher than the second endothermic peak temperature (softening point). That is, the low melting point glass component applied to the composite composition of the present invention preferably has a lower softening point and a higher crystallization start temperature. Thereby, the fluidity | liquidity of the composition at low temperature improves. In the conventional glass component, the lowering of the softening point is often accompanied by the lowering of the crystallization start temperature, but in the present invention, the second additional component of 0.1 mol% or more and 2.0 mol% or less, etc. As a result, the softening point can be lowered and the crystallization start temperature can be increased at the same time.

Here, the definition of the characteristic temperature in the present invention will be described. In the present invention, the characteristic temperature of the low melting glass component was measured by DTA. FIG. 1 shows a typical DTA curve of the glass component. In general, DTA as a glass component uses glass particles having a particle size of several tens of μm, and further uses high-purity alumina (α-Al ₂ O ₃ ) particles as a standard sample, and is 5 ° C./min in the atmosphere. Measured at a rate of temperature rise of. As shown in FIG. 1, the first endothermic peak start temperature is the transition point T _g , the endothermic peak temperature is the yield point T _d , the second endothermic peak temperature is the softening point T _s , and the exothermic peak start temperature due to crystallization. Is the crystallization start temperature T _cry . In addition, each characteristic temperature in this invention points out the value calculated | required by the tangent method. The characteristic temperatures of T _g , T _d, and T _s can also be defined by the viscosity of the glass. T _g is 10 ^13.3 poise, T _d is 10 ^11.0 poise, and T _s is 10 ^{7. The} temperature corresponds to ⁶⁵ poise. Crystallization tendency has a T _cry, the size of the exothermic peak due to crystallization, i.e. be determined from the calorific value, the high temperature of T _cry, i.e. a temperature difference increases between T _s and T _cry, a decrease in heat of crystallization It can be said that this is a glass component that is difficult to crystallize when observed.

  The resin component in the composite composition of the present invention is a low-polarity resin component that does not have a hydroxyl group and an amino group, and any of thermosetting resins and thermoplastic resins can be applied as long as this condition is satisfied. In the absence of a polar group, the dielectric properties are low, and therefore, the resin component alone generally has low adhesion to different materials, metals, and inorganic materials. Moreover, when an electrothermal characteristic is required, it adds and uses an inorganic filler with respect to a resin component, However, Addition of an inorganic filler causes a further adhesive fall. In the present invention, a low-melting glass component that has a predetermined composition and is difficult to crystallize is employed, so that it can be combined with a low-polarity resin component. When the glass component is crystallized, it does not melt uniformly with the resin component, so that the sea-island structure as shown in FIG. 2 is not organized and the adhesive strength is reduced. Therefore, in the present invention, the adhesive strength of the composite composition is ensured by suppressing the crystallization of the glass component.

  Examples of applicable thermosetting resins include epoxy resins, phenol resins, urea resins, melamine resins, silicone resins, unsaturated polyester resins, polyurethane resins, and the like. Examples of thermoplastic resins include nylon, polyacetal, polysulfone, polyetherimide, polyamideimide, liquid crystal polymer, polytetrafluoroethylene, polychlorotrifluoroethylene, polyvinylidene fluoride, aromatic polyether, polyphenylene ether, poly Examples include ether ether ketone, polyphenylene oxide, polycarbonate, polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate, polyether sulfone, polyarylate, and polyoxybenzoyl polyester.

  Preferably, the resin component is any one or more selected from aromatic polyether, polyether ether ketone, polycarbonate, polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate, polyether sulfone, polyarylate, and polyoxybenzoyl polyester. including. Since these resin components have high heat resistance and excellent moldability, they are suitable as resin components for composite compositions.

  In addition, particularly preferably used resin components include those having polyphenylene ether in the molecular chain. Specific examples of such a resin component include a resin component having the partial structure shown below.

  In the composite composition of the present invention, the blending ratio of the low-melting glass component and the resin component can be appropriately set in consideration of the use of the composite composition and the like, and is not particularly limited. For example, low melting point glass component: resin component = 10: 90 to 90:10 (weight ratio) can be mixed and used in combination.

  The composite material composition of the present invention can further contain a conductive material. As an electroconductive material, any 1 or more types selected from silver, a silver alloy, copper, a copper alloy, aluminum, an aluminum alloy, tin, and a tin alloy can be included, for example.

  As an example, the composite material composition of the present invention can be used by preparing a paste in combination with a solvent.

  As the solvent, α-terpineol or butyl carbitol acetate can be preferably used, but is not limited thereto.

  A particularly preferable combination is a paste agent in which the conductive material is silver or aluminum and the solvent is α-terpineol.

  The paste can be prepared in various compounding ratios. For example, the low melting point glass component and the conductive material are blended in a ratio of 50:50 to 10:90 (volume ratio) so that the solid component content in the paste is 70% by mass to 80% by mass. It can be prepared by adding a resin component and a solvent. When the paste having the composition in the above range is fired and the cross section of the structure is observed, as shown in FIG. 2, the resin component 21 spreads in the interspersed voids, which is a characteristic after firing the low melting point glass component 22. A state close to the sea-island structure is obtained. As an example of a preferred paste composition, butyl carbitol is used as a solvent with respect to 75% by weight of a solid component prepared by mixing 60% by volume of silver, 25% by volume of a low melting glass component, and 15% by volume of modified polyphenylene ether (OP2St). The case where 25 weight% of acetate is mix | blended and used can be mentioned.

  Conventionally, when a glass component is used alone as a sealing material or an adhesive, the interspersed voids in FIG. 2 have caused a decrease in adhesion and adhesiveness. In the composite material composition of the present invention in which a predetermined resin component and a low-melting glass component are combined, the adhesiveness and adhesion can be improved compared to the low-melting glass component alone due to the reduction of the voids.

  Therefore, the composite material composition of the present invention is capable of adhering and adhering to copper, silver, aluminum, silicon, ferrite and other base materials during sealing and adhesion, and formation of conductive joints in addition to the above paste agent. It can be used as a sealing material or an adhesive for enhancing the properties. Moreover, the composite material composition of the present invention can make it possible to achieve both improvement in adhesiveness and improvement in heat dissipation and thermal conductivity, which has been a problem of conventional resin materials. Furthermore, the problem that the conventional resin material has a large electric resistance and a low gas barrier property can be solved. The composite composition of the present invention can be soldered or plated.

  Moreover, the composite material composition of the present invention is also applicable as a glass sealing material. Specifically, it can be used as a sealing material for display panels such as vacuum heat insulating multilayer glass panels, plasma display panels, organic EL display panels, fluorescent display tubes and the like applied to window glass and the like. Furthermore, it can also be applied as an adhesive in various electric and electronic parts such as solar cells, image display devices, multilayer capacitors, crystal resonators, LEDs (light emitting diodes), multilayer circuit boards, IC ceramic packages, and semiconductor sensors. .

EXAMPLES Hereinafter, although an Example and a comparative example demonstrate this invention further in detail, this invention is not limited to these.
In this example, assuming that the composite material composition is applied to a heat dissipation structure or a semiconductor module as an electronic component, a paste agent is prepared from the composite material composition, and the adhesiveness and heat conduction of the obtained paste agent are prepared. The rate was evaluated.

1. Preparation of paste for electronic parts Lead-free low-melting glass components G1 to G9 shown in Table 1 were prepared. The composition shown in Table 1 is a blending composition at the time of preparation of the low melting point glass component, and all the units are mol%. G1 to G7 have compositions within the scope of the present invention (Examples), and G8 to G9 have compositions outside the scope of the present invention (Comparative Examples). As the starting material, promotion Kagaku _V 2 _{O 5,} manufactured by Kojundo Chemical Laboratory TeO _2, manufactured by Wako Pure Chemical Industries, Ltd. _Ag 2 O, manufactured by Kojundo Chemical Laboratory BaO, manufactured by Kojundo Chemical Laboratory WO _3, high purity chemical Research Laboratory _P 2 _{O 5,} manufactured by Kojundo Chemical Laboratory _Y 2 _{O 3,} powder was used Kojundo Chemical Laboratory Ltd. _La 2 _{O 3,} and by Kojundo Chemical Laboratory _Al 2 _{O 3.}

  The powders of each starting material were weighed, blended and mixed so that the total amount was about 200 g, and put into a quartz glass crucible. Subsequently, the quartz glass crucible charged with the mixed powder is placed in a glass melting furnace and heated to 700 ° C. to 750 ° C. at a rate of temperature increase of about 10 ° C./min, so that the composition of the melt in the quartz glass crucible is uniform. In order to achieve this, the mixture was held for 1 hour while stirring with an alumina rod. Thereafter, the quartz glass crucible was taken out from the glass melting furnace, and the melt was poured into a stainless steel mold heated to around 120 ° C. in advance to prepare lead-free low melting glass components G1 to G9, respectively. Next, the prepared lead-free low-melting glass component was pulverized to about 10 μm. Table 2 summarizes the characteristics of the prepared lead-free low-melting glass components. In the item “Vitrification State” in Table 2, a state in which no diffraction peak is observed by X-ray diffraction of the prepared lead-free low-melting glass component is “pass”.

As is clear from the results in Table 2, in the lead-free low-melting glass components G1 to G7, the exothermic peak indicating crystallization disappears and the crystallization tendency is remarkably reduced. Meanwhile, G8 has a large heat of crystallization, also in _{G9, T cry} is being heated to a high temperature, the crystallization tendency is not possible to suppress as much as G1 to G7.

  Next, a lead-free low-melting glass component powder having an average particle size of 2 μm or less and Ag particles having an average particle size of 3.5 μm (large particles) and 1.5 μm (small particles) as a conductive material in a predetermined volume. The paste component for electronic parts was produced by adding a resin component and a solvent, mixing well, and knead | mixing so that it may mix | blend by ratio and the content rate of solid content may be 80 mass%. Modified polyphenylene ether (OPE2St) manufactured by Mitsubishi Gas Chemical was used as the resin component, and α-terpineol manufactured by Wako Pure Chemical was used as the solvent. Table 3 shows the composition of the prepared paste for electronic parts.

2. Evaluation of Adhesiveness FIG. 3 shows a method for preparing a sample for evaluating adhesiveness. First, a columnar substrate 31 having a height of 5 mm and having a bonding surface of φ5 mm was prepared (FIG. 3A). Next, the prepared paste for electronic components was applied to the joint surface of the columnar substrate 31 by a dispenser method. Then, it is dried at 120 ° C. to 150 ° C. in the atmosphere, put into an electric furnace, heated to 220 ° C. at a heating rate of 10 ° C./min in an inert gas (nitrogen) or in the atmosphere, and held for 15 minutes. After that, it was heated to a temperature 50 ° C. to 60 ° C. higher than the softening point of each low-melting glass component at the same rate of temperature rise, and held for 15 minutes. Subsequently, the joining surface 32 is placed on a plate-like base material 33 having a thickness of 3 mm to 5 mm, sandwiched between heat-resistant clips, and 270 ° C. at a temperature rising rate of 10 ° C./min in an inert gas (nitrogen) or in the atmosphere. Or it heated to 290 degreeC and produced the joined body by hold | maintaining for 15 minutes (FIG.3 (b)).

  About each produced joined body, the shear stress was measured. As the plate-like substrate, a copper or aluminum substrate was used. The shear stress was evaluated as “excellent” when the measured value was 30 MPa or more, “good” when 20 MPa to 30 MPa, “normal” when 10 MPa to 20 MPa, and “fail” when less than 10 MPa. . Table 4 shows the evaluation results of the shear stress.

  In the pastes of P1 to P9, by using a lead-free low-melting glass component that suppresses crystallization and OPE2St that is a low-polarity resin component, the shear stress is P10 paste that does not contain a resin component, and a low-melting point Compared to the P11 paste containing no glass component, an excellent tendency was exhibited. Moreover, although the paste agent of P12-P13 using the lead-free low melting-point glass component in which crystallization is not suppressed was a favorable shear stress, it did not become an excellent result. This is probably because the lead-free low-melting-point glass component that tends to crystallize cannot be melted uniformly with the resin component, and the formation of a sea-island structure becomes insufficient.

3. Evaluation of thermal conductivity A plate-like molded article having a diameter of 10 mm and a thickness of 2 mm was produced from each prepared paste using a hand press. The pressurization at this time was 500 kgf / cm ² . The produced compact is heated in an electric furnace at a heating rate of 10 ° C./min in the atmosphere to a temperature 50 ° C. to 60 ° C. higher than the softening point of the lead-free low-melting glass component, and held for 30 minutes to sinter The body was made. And the upper and lower surfaces of the produced sintered body were polished, and the thermal conductivity was measured by a xenon flash method. Table 4 shows the measurement results.

  In addition, the sample for thermal conductivity measurement which does not use the low melting-point glass component corresponding to P11 was produced as follows. First, 0.01 g of benzoyl peroxide manufactured by Tokyo Chemical Industry was added to 10 g of OPE2St and dissolved. Furthermore, Ag particles were added at a blending ratio shown in Table 3, and the mixture was made into a paste, poured into an aluminum cup having a diameter of 10 mm, and kept in a thermostatic bath at 150 ° C. for 2 hours to produce a cured product containing OPE2St and Ag particles. The produced cured product was polished, a sample having a diameter of 10 mm and a thickness of 2 mm was produced, and the thermal conductivity was measured.

  As shown in Table 4, the thermal conductivity of the pastes P1 to P9 was remarkably improved as compared with P11 consisting only of the resin component and Ag particles.

4). Evaluation of solder wettability A sample for evaluating solder wettability was manufactured by the same manufacturing method as that for evaluation of thermal conductivity. Soldering was performed on the surface of the plate-like molded body, and when it was wet, it passed, and when it was not wet, it was rejected.

  As shown in Table 4, in the pastes of P1 to P9, it was found that the wettability was acceptable and soldering was possible.

5. Evaluation of plating uniformity A sample for evaluating the uniformity of plating was prepared by the same manufacturing method as in the case of evaluation of thermal conductivity. When the surface of the plate-shaped molded body was uniformly plated, it was accepted, and when it was not uniform, it was rejected.

  As shown in Table 4, it was found that the P1-P9 paste agent can be uniformly plated. Further, it was found that the composite material composition of the present invention can be applied to both solder joining and plating techniques.

  The embodiment of the present invention has been described in detail above, but the specific configuration is not limited to this embodiment, and even if there is a design change or the like without departing from the gist of the present invention, It is included in the present invention.

21 resin component 22 low melting point glass component 31 columnar substrate 32 bonding surface 33 plate substrate

Claims (11)

A composite composition comprising a low melting glass component and a resin component having no hydroxyl group and amino group,
The low melting glass component _comprises V ₂ O 5, TeO ₂ and Ag ₂ O, and at the total content of _{V 2 O} 5, TeO 2 and Ag ₂ O in the low-melting-point glass component 78 mol% or more, and TeO content of ₂ and Ag ₂ O _is, the composite material composition is 1 to 2 times by molar ratio, respectively relative to the content of V 2 _{O 5.} 2. The composite composition according to claim 1, comprising as a first additional component any one or more selected from BaO, WO ₃ and P ₂ O ₅ in a low melting glass component in an amount of 0 to 20 mol%. As a second additional component, at least one selected from Y ₂ O ₃ , La ₂ O ₃ , Al ₂ O ₃ and Fe ₂ O ₃ is 0.1 mol% or more and 2.0 mol% or less in the low melting point glass component. The composite material composition according to claim 2.   The composite composition according to any one of claims 1 to 3, wherein a softening point that is a second endothermic peak temperature by differential thermal analysis of the low-melting glass component is 280 ° C or lower.   The composite material composition according to claim 4, wherein the low-melting-point glass component has a crystallization start temperature by differential thermal analysis that is 60 ° C. or more higher than the softening point.   The composite composition according to any one of claims 1 to 5, wherein the resin component comprises polyphenylene ether.   Claims in which the resin component contains any one or more selected from aromatic polyether, polyether ether ketone, polycarbonate, polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate, polyether sulfone, polyarylate and polyoxybenzoyl polyester Item 6. The composite composition according to any one of Items 1 to 5.   Furthermore, the composite material composition in any one of Claims 1-7 containing an electroconductive material.   The composite material composition according to claim 8, wherein the conductive material includes at least one selected from silver, silver alloy, copper, copper alloy, aluminum, aluminum alloy, tin, and tin alloy.   The paste agent containing the composite material composition in any one of Claims 1-9, and a solvent. The paste according to claim 10, wherein the solvent is α-terpineol or butyl carbitol acetate.

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