CN101154479B - Dielectric composition, capacitor and light wiring using the dielectric composition - Google Patents

Abstract

This invention is a paste composition containing an inorganic filler, a resin and a solvent, wherein the paste composition is characterized in that it contains one or more solvents of which boiling point is 160 DEG C or higher and an inorganic filler of which mean particle diameter is 5 m or smaller, and the total content of the solvent being 25 wt% or less based on the total amount of the paste composition, and relates to a dielectric composition containing an inorganic filler and resin, wherein the inorganic filler includes inorganic fillers of at least two kinds of mean particle diameter, and the greatest mean particle diameter of said mean particle diameters is 0.1-5 m and is 3 times or more to the minimum mean particle diameter. By this invention, it is possible to obtain a high dielectric constant composition of which linear expansion coefficient is low, and which has a large capacitance.

Description

Dielectric composition and capacitor that has used this dielectric composition and light wiring

The application is that application number is 200480009120.2, the applying date is on March 25th, 2004, denomination of invention is divided an application for the patent application of " paste composition and used the dielectric composition of this paste composition ".

Technical field

The present invention relates to a kind of as capacitor or have a dielectric composition that interlayer dielectic that the circuit material of capacitor function uses or light wiring material show excellent characteristic.

Background technology

In recent years, along with the miniaturization of electronic instrument, the high speed of signal or the development that high capacity requires, the densification that circuit block is installed is constantly progressive.But, also occurred electric noise increase, produce problem such as error in data.In order to suppress the generation of this electric noise, semiconductor device is stably worked, to provide the electrorheological of necessary amount to get important with the closer position of semiconductor device.For this purpose, under semiconductor device, disposing jumbo capacitor is effective as the decoupling capacitance device.

Therefore, as the method for configuration capacitor on printed circuit board, the method for the external capacitors such as (chip condenser) of configuring chip capacitor on printed circuit board is arranged also.But consider from the viewpoint of miniaturization, the method that adds inorganic filler in the internal layer of printed circuit board, make printed panel itself have the function of capacitor is favourable, known have use to be mixed with the method (spy open flat 5-57852 communique, spy open flat 6-85413 communique) of the complex of inorganic filler and resin as interlayer dielectic.But the dielectric constant of the complex that makes with said method is low, be about 10～20.

The composite dielectrics that contains inorganic filler can improve its dielectric constant by the addition that increases inorganic filler, but exists when the content of inorganic filler surpasses 50 volume %, even increase the problem that the content of inorganic filler can not improve dielectric constant.In addition, if in resin, mix the inorganic filler of a large amount of high-ks, then uprise, so need a large amount of solvents usually owing to viscosity.

Polyelectrolyte composition up to now is to carry out (spy opens flat 10-158472 communique) that desolventizing, curing make by the paste composition that will contain inorganic filler, resin and solvent.But, if the amount of the solvent that uses is too much, then produce stable on heating reduction that residual solvent causes, on the top layer, produce shortcoming such as space.

As the method that obtains high-k, known have add filler with 2 kinds or its above particle diameter, improve the filling rate of filler, improve the method (spy opens clear 53-88198 communique, and the spy opens the 2001-233669 communique) of dielectric constant thus.But, use therein filler, the average grain diameter of filler with maximum average grain diameter is very big, is 5 μ m or more than it, the thickness of this filler and the resulting complex of mixed with resin must not be not really thick, is about 300 μ m.

In addition, as the method that improves dielectric constant, the method for using the big inorganic filler of particle diameter is arranged.The dielectric constant of filler depends on the crystal structure of filler.Generally in inorganic crystal, as finding at barium titanate etc., anion and cationic position of centre of gravity deviation can be brought very big dielectric constant.As filler the time, if its particle diameter diminishes, then general crystal particles size also diminishes, and it is big that the surface energy of particle becomes, and is the energy of reduction system integral body, and the symmetry of crystal structure becomes higher.Because the symmetry of crystal structure is high more, then the position deviation of anion and cationic center of gravity is more little, so dielectric constant diminishes.Therefore, by using the big filler of particle diameter, can improve dielectric constant.Particularly in the barium titanate, this effect is obvious.For example, have use average grain diameter be the barium titanate of 15 μ m as filler, use the example (spy opens flat 8-293429 communique) of ethyl carbitol (boiling point is 202 ℃).But because the particle diameter of filler is big more, the specific area of filler is more little, so even use the high solvent of boiling point, the precipitation thinner during heating also can be carried out under lower temperature in short time.Like this, utilize the resin of the contraction that is accompanied by system integral body or moving of filler, make and carry out desolventizing, therefore produce a large amount of spaces with very fast speed.The generation in space is the reason that dielectric constant reduces.If use the big filler of average grain diameter, though then the dielectric constant of filler itself becomes big, even the use high boiling solvent can not suppress the generation in above-mentioned space, dielectric constant is 52 as a result, can not obtain very big value.In addition, owing to use the filler (spy opens flat 8-293429 communique) of the big average grain diameter of 15 μ m, thus can only obtain the very thick thickness of 25 μ m, so static capacity density is 1.8nF/cm ², very little.

On the other hand, for realizing the small-sized slimming of inner system of installing, not only memory, mix the also development rapidly of exploitation of the high density SiP (package system) of the LSI carry the multiterminal subnumber, in be loaded on capacitor strong request slimming among this SiP, this capacitor must be at 10 μ m or below it with the thickness of interlayer dielectic.Therefore, prior art can not satisfy 10 μ m or its following slimming requirement, is difficult to adapt to the demand aspect the quick slimming that increases in the high performance of portable sets such as mobile phone.

And then, because the static capacity of capacitor is inversely proportional to the thickness of interlayer dielectic, so, preferably make the thickness attenuation of interlayer dielectic from the viewpoint of the big direct capacitance quantification of capacitor.

In addition, as the desired important fundamental characteristics of interlayer dielectic, can enumerate low linear expansion coefficient.The coefficient of linear expansion of resin itself is 50ppm/ ℃ or more than it, with the metal that constitutes wiring layer for example the coefficient of linear expansion of copper (17ppm/ ℃) compare very big.Therefore, when only using the interlayer dielectic that constitutes by resin, because and the difference of the coefficient of linear expansion between the wiring layer, and produce troubles such as splitting that stress causes or cloth thread breakage.Relative therewith, if make inorganic filler and resin compoundedization, then can reduce coefficient of linear expansion, therefore when the complex that is mixed with inorganic filler and resin in use is as interlayer dielectic, can make its value near the coefficient of linear expansion of wiring layer.But, in existing method, can not make the fully high fillingization of inorganic filler, can not make it to drop to basic coefficient of linear expansion near wiring layer.

Summary of the invention

In view of the foregoing, the present invention is a purpose to obtain the low high dielectric composition of coefficient of linear expansion, and then, provide a kind of dielectric composition of having realized sufficient slimming and light wiring material to be loaded on big static capacity capacitor interlayer dielectic among the high density SiP in being used as.

Promptly, the present invention is a kind of paste composition, it is that to contain inorganic filler, resin and solvent boiling point be the paste composition that the above solvent of 160 ℃ or its forms, it is characterized in that, having a kind or its above solvent boiling point is 160 ℃ or its above solvent, average grain diameter with filler is the following inorganic filler of 5 μ m or its, and the total solvent amount accounts for 25 weight % of paste composition total amount or below it.

In addition, another form of the present invention is a kind of dielectric composition, it is the dielectric composition with inorganic filler and resin, it is characterized in that, inorganic filler has 2 kinds of average grain diameters at least, average grain diameter maximum in the above-mentioned average grain diameter is 0.1～5 μ m, and with respect to minimum average particle diameters, maximum average grain diameter is its 3 times or more than it.

According to the present invention, can easily obtain dielectric constant very high, be 50 or its above dielectric composition.And then, because composition of the present invention has the low linear expansion coefficient close substantially with the coefficient of linear expansion of wiring metal, so when using as interlayer dielectic, be difficult for to produce and wiring layer between peel off or trouble such as cloth thread breakage the capacitor that can obtain to have high reliability.And then, can easily obtain to have the film of rerum natura of thickness, the homogeneous of homogeneous.Because it is fit to big static capacity, so applicable to the interior circuit base material interlayer dielectic that is loaded on the capacitor among the high density SiP or has the function of capacitor.

Embodiment

Paste composition of the present invention is the paste composition that comprises inorganic filler, resin, solvent, it is characterized in that, average grain diameter with filler is 5 μ m or its following inorganic filler, contain solvent boiling point at 160 ℃ or solvent more than it, and the total solvent amount accounts for 25 weight % of paste composition total amount or below it.

In addition, the present invention is the dielectric composition with inorganic filler and resin, it is characterized in that containing the inorganic filler that has 2 kinds of average grain diameters at least, the average grain diameter that wherein has the inorganic filler of maximum average grain diameter is 0.1～5 μ m, with respect to minimum average particle diameters, maximum average grain diameter is its 3 times or more than it.

Total solvent amount in the paste composition of the present invention is necessary for 25 weight % of paste composition total amount or below it.Be preferably 20 weight % or below it, more preferably 10 weight % or below it.In addition, be preferably 1 weight % or more than it.When quantity of solvent is 25 weight % or its when following, the dielectric constant of dielectric composition can be improved in the space that the solvent evaporates in the time of can suppressing drying causes.In addition, the pore volume of reason that becomes moisture absorption owing to meeting is little, changes so can reduce the rerum natura that the influence because of humidity, moisture produces.And then, make the preservation durability good.If quantity of solvent is more than 25 weight %, then in removing the drying process and hot curing operation that desolvate, the gap increases, and the situation that the dielectric constant of dielectric composition reduces is a lot.Because when quantity of solvent less than 1 weight %, solvent seldom, so the infringement paste composition viscosity and homogeneity.

In addition, follow the raising of the pack completeness of inorganic filler, the above-mentioned influence that is produced by quantity of solvent becomes big, and when the 85 weight % that the solid formation that inorganic filler accounts in the paste composition to be contained divides or its were above, effect of the present invention was big especially.

The solvent that uses among the present invention, the boiling point that must have a kind at least are 160 ℃ or more than it.Be preferably 180 ℃ or more than it, more preferably 200 ℃ or more than it.When the boiling point of solvent is 160 ℃ or its when above, can suppress the generation in space, improve the dielectric constant of dielectric composition.If boiling point is lower than 160 ℃, then because the evaporation rate of solvent is fast,, the gap is increased so the material can not catch up with heat treatment the time moves the densification that causes, the situation that the dielectric constant of dielectric composition is reduced is a lot.In addition, the solvent that uses among the present invention is preferably boiling point at 300 ℃ or below it, more preferably at 280 ℃ or below it.If boiling point is higher than 280 ℃, the processing that then is used for desolventizing becomes needs high temperature, Yin Gaowenization to cause resin to decompose, and causes dielectric property variation etc.In addition, if greater than 300 ℃, then the decomposition of resin is fiercer, causes mechanical strength to descend.The employed solvent of paste composition of the present invention can only use boiling point at 160 ℃ or a kind of solvent more than it, if but contain boiling point at 160 ℃ or solvent more than it, then also can contain other solvents.

Boiling point has mesitylene at 160 ℃ or solvent more than it, acetonyl acetone, methyl cyclohexanone, isobutyrone, acetophenone, dimethyl sulfoxide (DMSO), gamma-butyrolacton, isophorone, diethylformamide, dimethylacetylamide, the N-methyl pyrrolidone, butyrolactam, the acetate glycol ester, 3-methoxyl group-3-methyl butanol and acetic acid esters thereof, 3-methoxyl group butylacetic acid ester, acetate 2-ethylhexyl, oxalate, diethyl malonate, maleate, the isobutyl carbonate propylene glycol ester, butyl cellosolve, ethyl carbitol etc.

Among the present invention, preferred use contains the solvent of ester structure, further preferably contains the solvent of lactone structure.Most preferred solvent is a gamma-butyrolacton.Boiling point among the present invention is meant at 1 atmospheric pressure, promptly 1.013 * 10 ⁵N/m ²Pressure under boiling point.The mensuration of boiling point can use technique known to carry out, and is not particularly limited, but for example can measures by the ebulliometer that uses Swietoslawski.

In addition the solvent that uses among the present invention can suitably be selected the solvent of dissolving resin.Solvent for example preferably uses, methyl cellosolve, N, dinethylformamide, methyl ethyl ketone, two

Alkane, acetone, cyclohexanone, cyclopentanone, isobutyl alcohol, isopropyl alcohol, oxolane, toluene, chlorobenzene, trichloroethylene, benzylalcohol, methoxy butanols, ethyl lactate, propylene glycol monomethyl ether and acetic acid esters thereof etc. and contain in them a kind or its above ORGANIC SOLVENT MIXTURES.

The shape of inorganic filler can list spherical, approximate spherical, oval spherical, needle-like, tabular, flakey, bar-shaped etc., is preferably sphere or almost spherical especially.Because spherical or approximate spherical filler specific area minimum, so when filling, be difficult for taking place filler aggegation or Resin Flow reduction etc.Can use a kind in them separately, or mix use 2 kinds or more than it.

For obtaining low linear expansion coefficient and high-k, preferably in resin, contain these inorganic fillers with high fill-ratio.

As the general organic resin that uses of interlayer dielectic, for example polyimides has 30～50ppm/ ℃ coefficient of linear expansion, and epoxy resin has 50ppm/ ℃ or its above coefficient of linear expansion.This with wiring metal for example the coefficient of linear expansion of copper be 17ppm/ ℃ and compare, be very large, but, coefficient of linear expansion descended by mixing inorganic filler.

In addition, in the dielectric composition that comprises inorganic filler and resin, the dielectric constant of this dielectric composition meets the derivation formula of the dielectric constant of complex, so-called following logarithm mixes rule (1) (ceramic material grammar of science (using version), interior Tian Laohe garden Xin She, translate W.D.Kingery, Xiao Song and Tibetan etc., p912).The content of inorganic filler with high-k is high more, and the dielectric constant of the dielectric composition that obtains is high more.

$\log \mathrm{\ϵ}=\underset{i}{\mathrm{\Σ}}{V}_i\·\log {\mathrm{\ϵ}}_i---\left(1\right)$

ε: the dielectric constant of complex

ε _i: the dielectric constant of each composition of complex

V _i: the percentage by volume of each composition of complex

For containing inorganic filler with high fill-ratio in resin, the preferred mixing used the inorganic filler with 2 kinds or its above different average grain diameters.When filling the filler of single particle size, be spherical or approximate when spherical particularly at filler, fill if carry out high density, then will between filler and filler, produce the space of rhombus, in this space, can not enter other fillers.But if filler smaller or equal to this space is arranged, then it can further enter this space, can easily improve filling rate.

In the inorganic filler that the present invention contains, the difference of average grain diameter of average grain diameter and the inorganic filler with minimum average particle diameters of inorganic filler with maximum average grain diameter is than being the bigger the better, maximum average grain diameter is preferably with respect to minimum average particle diameters, be 3 times or more than it, more preferably 5 times or more than it.If difference is than very little, then little filler is difficult for entering effectively the space between the big filler.On the other hand, if difference is big than very, the easy aggegation that becomes of then little filler, dispersion stabilization reduction.The difference ratio is preferably at 30 times or below it, further preferably at 10 times or below it.

Under the situation of using the inorganic filler have 2 kinds of average grain diameters at least, this cumulative volume Vb of cumulative volume Va and the inorganic filler with minimum average grain diameter with inorganic filler of maximum average grain diameter preferably satisfies 0.05≤Vb/ (Va+Vb)≤0.5.That is, the amount of little filler is in volume ratio, be preferably the filler total amount 5% or it is above and less than 50%.Less than 5% o'clock, can not obtain substantially to enter the space and the effect that improves loading, more than or equal to 50% o'clock, the shared volume of little filler is greater than the volume of the hole that is made of big filler, and the effect that enters, increases loading mutually diminishes.

Except these big fillers, little filler, further also can mix the filler of other particle diameters, by selecting suitable particle diameter and proportioning,, also can obtain to improve the effect of filling rate even mix 3 kinds or its above filler.

The inorganic filler that uses among the present invention contains the inorganic filler that has 2 kinds of different average grain diameters at least, and the average grain diameter that wherein preferably has the inorganic filler of maximum average grain diameter is 5 μ m or below it.2 μ m or below it more preferably, more preferably 1 μ m or below it.In addition, be preferably 0.1 μ m or more than it, 0.2 μ m or more than it more preferably, more preferably 0.3 μ m or more than it.Herein, the average grain diameter of inorganic filler that has maximum average grain diameter when use is greater than the filler of 5 μ m, and when wanting to make thickness and being 10 μ m or its following capacitor, filler is outstanding from the surface of film easily, therefore is difficult to obtain stable dielectric characteristics.In addition, when the average grain diameter that has an inorganic filler of maximum average grain diameter when use was 2 μ m or the filler below it, the filler of filler dispersion liquid is free settling not.And then when the average grain diameter that has an inorganic filler of maximum average grain diameter in use was 1 μ m or the filler below it, in long preservation, filler is free settling not, and preservation condition is unrestricted.On the other hand, when expecting the big material of dielectric constant, when the average grain diameter of maximum during less than 0.1 μ m, because the specific area of these fillers is big, so the symmetry of crystalline texture uprises easily, be difficult to obtain the high-k phase, cause the dielectric constant of dielectric composition to reduce.In addition, if maximum average grain diameter is 0.2 μ m or more than it, then the filler surface area diminishes, filler disperses paste to be difficult to aggegation, and viscosity changes little, be not vulnerable to mixing, disperse or the influence of coating processing.And then, if have the average grain diameter of the inorganic filler of maximum average grain diameter and be 0.3 μ m or more than it, the average grain diameter that then has the inorganic filler of maximum average grain diameter compares greatly with the differing from of average grain diameter of the inorganic filler with minimum average particle diameters, so filling rate is more stable.

In addition, in the present invention, the average grain diameter with inorganic filler of minimum average particle diameters is preferably 0.01～0.1 μ m.And then, more preferably use the inorganic filler of 0.04～0.06 μ m.In addition, owing to must make maximum average grain diameter and minimum average particle diameters have poor ratio, can in above-mentioned scope, suitably select according to maximum average grain diameter so have the inorganic filler of minimum average particle diameters.The difference of average grain diameter and the average grain diameter of the inorganic filler with maximum average grain diameter of inorganic matter with minimum average particle diameters can improve filling rate when big.According to this reason, consider to have the average grain diameter of the inorganic filler of minimum average particle diameters from the scope that the average grain diameter of inorganic filler with maximum average grain diameter is suitable, be preferably 0.1 μ m or below it, more preferably 0.06 μ m or below it.When the average grain diameter of the inorganic filler with minimum average particle diameters is 0.04 μ m or its when above, the aggegation again after difficult the dispersion, the dispersion stabilization of paste is good.In addition, the average grain diameter of inorganic filler with minimum average particle diameters is difficult between these fillers the secondary aggegation takes place, thereby dismisses agglutination body easily further when 0.01 μ m or its are above, is easy to disperse.

The mensuration of the average grain diameter that contains in paste composition of the present invention and the dielectric composition can followingly be carried out, form the dielectric composition film, the ultra-thin section that obtains along the film thickness direction cutting film cross section of this film is carried out XMA measures and transmission electron microscope (TEM) observation.Inorganic filler is different to the transmitance of electron ray with resin, and therefore in the tem observation image, inorganic filler and resin can utilize the difference of contrast to discern.Determining of each inorganic filler when using multiple inorganic filler, the crystalline texture analysis that can utilize the elementary analysis measured based on XMA and electron ray diffraction image to observe is carried out.With this, try to achieve the area distributions of the filler and the resin of such acquisition by graphical analysis, the cross section of inorganic filler can be approximately circular, calculate particle diameter by planimeter.The evaluation of particle diameter is as long as be the TEM image of 5000 times and 40000 times to multiplying power.Being the particle size distribution representing with the histogram of 0.1 μ m scale in 5000 times the TEM image to be calculated in multiplying power, being to represent the particle size distribution that calculated with the histogram of 0.01 μ m scale in 40000 times the TEM image in multiplying power, is that peaked other intermediate value of level is as average grain diameter with the number of degrees.So-called " having 2 kinds of average grain diameters at least " means among the present invention, has 2 or its this above maximum,, has 2 or its above maximum in the particle size distribution of the inorganic filler that contains in the composition that is.In addition, as the evaluation method of particle size distribution, also can use scanning electron microscope (SEM) to replace above-mentioned method TEM.

In addition,, can utilize the electrophoretic light scattering method etc. of Doppler effect of the dynamic light scattering method that shakes, the scattered light when measuring the filler electrophoresis of the scattered light that the Brownian movement of measuring filler produces, measure average grain diameter as additive method.As laser diffraction, diffuse transmission type particle size distribution device, rise abruptly a made LA-920 of making or the system SALD-1100 of Shimadzu Seisakusho Ltd., day machine dress system MICROTRAC-UPA150 etc. are for example arranged.

As the dielectric property of inorganic filler, preferably using dielectric constant is 50～30000 inorganic filler.If the use dielectric constant then can not obtain the enough big dielectric composition of dielectric constant less than 50 inorganic filler.In addition, dielectric constant greater than 30000 inorganic filler in, the temperature characterisitic of dielectric constant has the tendency of variation, and is therefore not preferred.Here the dielectric constant of so-called inorganic filler is meant, is material powder with the inorganic filler, the dielectric constant of the sintered body that heats, burns till and obtain.The dielectric constant of sintered body is measured according to for example following order.The binding resin that inorganic filler and polyvinyl alcohol is such, organic solvent or water mix, and make the composition of pasty state, are filled into then in the grain forming device, carry out drying, obtain the graininess solid content.By this graininess solid content is for example being burnt till about 900～1200 ℃, can decompose and remove binding resin, the sintering inorganic filler obtains the sintered body that only is made of inorganic constituents.At this moment, the space of sintered body must be enough little, and the voidage that is calculated by solid density and actual density is necessary for 1% or below it.On this sintered body particle, form upper/lower electrode,, calculate dielectric constant according to the measurement result of static capacity and size.

Inorganic filler can list barium titanate class, metatitanic acid barium zirconate class, strontium titanates class, calcium titanate class, bismuth titanates class, magnesium titanate class, barium neodymium titanate class, barium titanate tin class, magnesium niobic acid barium class, magnesium barium tantalate class, lead titanates class, lead zirconates class, lead zirconate titanate class, lead niobate class, magnesium lead niobate class, nickel lead niobate class, lead tungstate class, artificial schellite class, magnesium lead tungstate class, titanium dioxide class etc.So-called barium titanate class is meant that containing with the barium titanate is the general name of the solid solution of fertile material, and described barium titanate is to replace a part of element of barium titanate crystallization inside or make other elements enter the barium titanate that forms in the crystalline texture with other elements.Other metatitanic acid barium zirconate classes, strontium titanates class, calcium titanate class, bismuth titanates class, magnesium titanate class, barium neodymium titanate class, barium titanate tin class, magnesium niobic acid barium class, magnesium barium tantalate class, lead titanates class, lead zirconates class, lead zirconate titanate class, lead niobate class, magnesium lead niobate class, nickel lead niobate class, lead tungstate class, artificial schellite class, magnesium lead tungstate class, titanium dioxide class all are the general name with the solid solution of the fertile material of respectively doing for oneself equally.

Preferred especially the filler that uses with Ca-Ti ore type crystalline texture or composite perofskite type crystalline texture.Can use a kind in them separately, or mix use 2 kinds or more than it, from the viewpoint of dielectric property, the inorganic filler that preferably has 2 kinds of different average grain diameters at least is same chemical composition.Particularly in order to obtain to have the high dielectric-constant dielectric composition, from taking into account the viewpoint of commercial convenience, the preferred compound that mainly constitutes that uses by barium titanate.But, in order to improve dielectric property, temperature stability, also can add displacement agent (shifter) on a small quantity, retardant (depressor) uses.

The manufacture method of inorganic filler can list, methods such as solid reaction process, hydrothermal synthesis method, supercritical water thermal synthesis method, sol-gel process, oxalate method.As the manufacture method of inorganic filler,, preferably use solid reaction process or oxalate method from the viewpoint of high-k and quality stability with maximum average grain diameter.In addition, have the manufacture method of the inorganic filler of minimum average particle diameters,, preferably use in hydrothermal synthesis method, supercritical water thermal synthesis method, the sol-gel process any from carrying out the reason of small particle diameterization easily.

Ratio as inorganic filler that contains in paste composition of the present invention and the dielectric composition and resin, be preferably the total volume of the cumulative volume that cumulative volume and resin with respect to inorganic filler form branch admittedly, the ratio Vf of inorganic filler satisfies 50%～95%.More preferably 70%～90%.When inorganic filler containing ratio Vf be 50% or its when above, can obtain enough big dielectric constant, obtain less coefficient of thermal expansion.In addition, when inorganic filler containing ratio Vf be 70% or its when above, use the effect of the inorganic filler that has 2 kinds of average grain diameters at least to become obviously, can obtain big dielectric constant.On the other hand, when inorganic filler containing ratio Vf be 95% or its when following, but the inner space that produces of composite inhibiting can obtain enough big dielectric constant, the hydroscopicity that the space causes is little, rerum natura is not vulnerable to the influence of moisture, humidity.In addition, when inorganic filler containing ratio Vf be 90% or its when following, after promoting the PCT (pressure cooker testing PressureCooker Test) of test as durability, adhesiveness is difficult for reducing.

In addition, the resin that uses among the present invention can be selected from any of thermoplastic resin, heat-curing resin.

Thermoplastic resin can use for example polyphenylene oxide, polyphenylene sulfide, polyether sulfone, Polyetherimide, liquid crystal polymer, polystyrene, polyethylene, fluororesin etc.

In addition, heat reactive resin can use for example epoxy resin, phenol resin, silicone resin, polyimides, acrylic resin, cyanate ester resin, benzocyclobutane olefine resin etc., can use the resin of the insulating barrier that is used in printed circuit board usually in addition.Consider from aspects such as scolding tin thermal endurances, preferably use heat-curing resin, particularly consider, preferably use epoxy resin from aspects such as hot curing shrinkage, viscosity.

Here, so-called epoxy resin is meant, has the resin of the prepolymer that contains 2 or its above epoxy radicals (oxirane ring) in the molecular structure.From the viewpoint of dielectric property, prepolymer preferably has biphenyl backbone or bicyclopentadiene skeleton.In addition, also can have curing agent, curing agent can use curing agent such as phenol novolac resin, bisphenol A-type novolac resin, amino triazine compound, naphthol compound.And then, can also add curing accelerators such as metal chelate compound such as triphenylphosphine, benzimidazoles compound, three (2, the 4-glutaric acid) cobalt.

Paste composition of the present invention can obtain by inorganic filler is dispersed in the resin.For example, can utilize following method to make, that is, inorganic filler be joined in the resin solution, mix the method for dispersion; Or inorganic filler is dispersed to makes dispersion liquid in the appropriate solvent in advance, discharge method (let down) method that this dispersion liquid is mixed with resin solution etc.In addition, disperse the method for inorganic filler to be not particularly limited in subtend resin or the solvent, for example, can use methods such as ultrasonic wave dispersion, ball mill, roller mill, emulsify at a high speed dispersion machine (Network レ ァ ミ ッ Network ス), homogenizer, medium dispersion machine, particularly consider, preferably use ball mill, homogenizer from dispersiveness.

When disperseing inorganic filler,, also can carry out the surface treatment of inorganic filler for example, the interpolation of dispersant, the interpolation of surfactant, the interpolation of solvent etc. for improving dispersiveness.As the surface treatment of inorganic filler, except the processing that utilizes various coupling agents, aliphatic acid, phosphates etc. such as silanes, titanium class, aluminium class, also can list rosin processing, acidic treatment, basic treatment etc.In addition, as the example that adds dispersant, can list the dispersant etc. that phosphoric acid, carboxylic acid, aliphatic acid and their ester class etc. have acid group, preferred especially the compound that uses with phosphate skeleton.In addition, also can list the surfactant that adds nonionic, cationic, anionic, polybasic carboxylic acid etc. wetting agent, two affinity substance, have the substituent resin of high spatial steric hindrance etc.In addition, during dispersion or the polarity of the system after disperseing can control by adding solvent.In addition, the pasty state combination also can be according to necessary stabilizer, dispersant, sagging inhibitor, plasticizer, the antioxidant etc. of containing.

The content that the solid formation that inorganic filler contains in paste composition of the present invention is occupied in dividing is preferably 85 weight %～99 weight %, 90 weight % or more than it more preferably, more preferably 94 weight % or more than it.If the content of inorganic filler at 85 weight % or more than it, then can easily improve the dielectric constant of composition.Among the present invention, follow the increase of the containing ratio of inorganic filler, can obtain having the high dielectric-constant dielectric composition, if containing ratio is 99 weight % or below it, the mouldability when then making film becomes easily, controls the dispersion of inorganic filler easily.In addition, the so-called solid branch that forms is meant the summation of inorganic filler and resin and other additives etc.

Dielectric composition of the present invention is to contain inorganic filler, resin and the dielectric composition that forms, and the amount of inorganic filler is 85～99 weight % of the solid formation branch total amount that contains in the dielectric composition, and voidage is 30 volume % or below it.

As the method that obtains dielectric composition of the present invention, for example can list, at first be manufactured on the paste composition that has mixed inorganic filler in the resin, this paste composition is coated on certain lining body (for example substrate), carry out desolventizing, curing, obtain the method for dielectric composition thus.At this moment, as the method for solidifying, can list the curing that utilizes heat, light etc.But, because dielectric composition of the present invention is not sintered body, thus there is no need to make resin to decompose fully, remove, preferably in the heat resisting temperature scope of electronic unit, for example 500 ℃ or the temperature below it heat.

The voidage of dielectric composition must be at 30 volume % or below it, preferably at 20 volume % or below it, further preferably at 10 volume % or below it.When voidage greater than 30% the time, inorganic filler shared ratio step-down in membrane volume is difficult to obtain dielectric constant and is 50 or its above dielectric composition.In addition, owing to produce reduction or the increase of leakage current, the reduction of bending strength etc. of insulation resistance, therefore not preferred.

Here, as making voidage reach 30 volume % or the method below it, can be by for example suitably selecting inorganic filler, resin, solvent to realize in from above the material, but by making paste composition contain a kind of boiling point at least is 160 ℃ or solvent more than it, and, make the total solvent amount be the paste composition total amount 25% or below it, can be easy to realize above-mentioned purpose.

In addition, be 20 volume % or below it for example in order to make voidage, if make paste composition contain a kind of solvent at least, then can make voidage reach 20 volume % or below it with lactone structure.In having the solvent of lactone structure, gamma-butyrolacton most preferably.

The assay method of the voidage of dielectric composition, can come suitable selection gas adsorption method, mercury penetration method, positron null method, small angle x-ray scattering (SAXS) method etc. according to purposes, but in the present invention, according to the order of following (1)～(3), obtain voidage by the density of high dielectric composition.

(1) in weighing be coated with paste composition, desolventizing, curing, the weight of the resulting dielectric composition of weighing on the setting substrate of weight.

(2) if establishing the weight of substrate is W1, the weight of substrate and dielectric composition is W2, and dielectric density is D, and volume is V, then the density D of dielectric composition=(W2-W1)/V.

(3) use thermogravimetric amount determining device (TGA), make this dielectric composition in air atmosphere with 10 ℃/minute of programming rates, be warming up to 900 ℃, keep taking off in 30 minutes adhesive treatment, measure the ratio that inorganic filler and resin contain in dielectric composition at 900 ℃.If the volume of inorganic filler is Wc, proportion is ρ c, and the volume of resin is Wp, and proportion is ρ p, and when voidage was P, voidage P can try to achieve by following formula.Voidage P (volume %)={ (V-Wc/ ρ c-Wp/ ρ p)/V} * 100.

Paste composition of the present invention is preferably coated on the lining body (for example substrate), carries out desolventizing, curing, and forms dielectric composition.As paste composition being coated the coating process of lining on the body, there is no particular restriction, can list for example spin coating, silk screen printing, blade coating, mould and be coated with etc.Like this, come the film of coating is carried out removing of solvent or hot curing, can be easy to obtain dielectric composition by using heaters such as electric hot plate, baking oven.

The lining body of coating paste composition can be selected from organic class substrate for example, mineral-type substrate with these substrates dispose the material of constituent material of circuit.As the example of organic substrate, can list flexible substrates such as heat-resisting thermoplasticity substrate such as compound copper plate pressing plate, polyetherimide resin substrate, polyether ketone resin substrate, polysulfones resin substrate, polyester copper plating film substrate, polyimides copper plating film substrate such as glass basis material copper plate pressing plate, glass nonwoven fabrics epoxy copper plate pressing plate such as glass cloth epoxy copper plate pressing plate.

In addition, the example of mineral-type substrate can list metal species substrates such as ceramic substrates such as aluminum oxide substrate, aluminium nitride substrate, silicon carbide substrate, aluminium base substrate, iron-based substrate.The example of the constituent material of circuit, can list the conductor of metals such as containing silver, gold, copper, contain mineral-type oxide etc. resistance, contain glass-like materials and/or resin etc. low-dielectric, contain resin or inorganic filler etc. high dielectric, contain insulator of glass-like materials etc. etc.

Form to dielectric composition of the present invention is not particularly limited, and can select membranaceously, bar-shaped, spherical etc. according to purposes, is preferably membranaceous especially.Here so-called film also comprises film, thin slice, plate, particle etc.Certainly, also can be according to the via hole that is formed for conducting, adjust impedance or static capacity or internal stress or give purposes such as heat release function and form figure.

Thickness when dielectric composition uses as film can be set in arbitrarily in the scope that satisfies the desired value of static capacity, is preferably 0.5 μ m～20 μ m.2 μ m～20 μ m more preferably.For guaranteeing the big static capacity as capacitor, the thickness of film is got over Bao Yuehao, but when thinner than 0.5 μ m, is easy to generate pin hole etc., is difficult to obtain electric insulation.In addition, when 2 μ m or its were above, behind the PCT (Pressure Cooker Test) that carries out as durable promotion experiment, dielectric loss angle tangent was difficult to increase.In addition,, then, need big dielectric constant, and be difficult to improve packing density for obtaining sufficient capacitor performance if thickness surpasses 20 μ m.

There is no particular restriction to the purposes of paste composition of the present invention and dielectric composition, but except for example being used in, with outside the interlayer dielectic, also can be used for interlayer dielectic, the frequency filter, wireless of multilager base plate as the interior capacitor of the printing circuit board of high dielectric constant layer with multiple electronic unit, devices such as antenna, electromagnetism guard shield, light wiring materials.

Dielectric composition of the present invention is preferably used as the capacitor interlayer dielectic.To using dielectric composition to form the method for capacitor, be not particularly limited with interlayer dielectic.For example, as mentioned above, can be by after forming high dielectric on the substrate, form suitable electrode and obtain.

As the static capacity of the capacitor that uses dielectric composition of the present invention to produce, preferably at 5nF/cm with the unit are of interlayer dielectic ²Or in its above scope.Further preferably at 10nF/cm ²Or in its above scope.When static capacity less than 5nF/cm ²The time, under situation about using, can't fully carry out and the separating of the power supply class of entire system as the decoupling capacitance device, can't give full play to the function of decoupling capacitance device.

On circuit design, the little side of difference in the variations in temperature of preferred static capacity, the face.For variations in temperature, be preferably as far as possible for a short time, for example, preferably satisfy X7R characteristic (rate of temperature change of the static capacity in the time of-55～125 ℃ is in ± 15%).Difference in the face of static capacity, being preferably with respect to mean value is 5% or (mean value of the mean value of static capacity-5%≤static capacity≤static capacity+5%) below it.

In addition, for reducing the electrical loss of power supply, the dielectric loss angle tangent of capacitor is preferably in 0.01～5% scope, more preferably in 0.01～1% the scope.Here, electrical characteristics such as static capacity, dielectric loss angle tangent are the measured value of frequency number when being 20k～1GHz.

Dielectric composition of the present invention also is suitable as the light wiring material and uses.So-called light wiring material is, the signal conduction between separately such as LSI, module, distribution board is not carried out with the common signal of telecommunication, and the wiring of the mode of carrying out with light signal.When on installation base plate or within it portion forms the light wiring, adopt the high layer of refractive index to be refracted the structure of the low layer of rate in the middle of being sandwiched in.Also but usage space replaces the low layer of refractive index.When using as the light wiring material, diminish with scattering of light owing in the light wiring, carry out the signal conduction of waveguide, be important so use is compared enough little inorganic filler with its light wavelength, be preferably 1/4 or its following particle diameter of light wavelength.In addition, the selection of the selection by the inorganic filler material, content, resin material can be controlled temperature dependency, the coefficient of thermal expansion of refractive index, refractive index.Form the wide range of selection of the baseplate material of light wiring layer thus, not only can use the substrate that constitutes by inorganic material such as the silicon of present use or potteries, the substrate that also can use organic material to constitute.

Below, embodiments of the invention are described, but the present invention is not subjected to their qualification.

Embodiment 1

Use homogenizer ice-cooled 0.5 μ m), 18 weight portion gamma-butyrolactons mix and disperseed 1 hour, obtain dispersion liquid A-1 down with 323 weight portion barium titanate fillers (Sakai chemistry (strain) system, BT-05, average grain diameter:.Mix 10 weight portion epoxy resin (Japanese chemical drug (strain) system, EPPN 502H), 10 weight portion phenol novolac resins (big Japanese ィ Application キ industry (strain) system, TD-2131), ((strain) system is learned in northern Xinghua to 0.6 weight portion curing accelerator, triphenylphosphine), 20 weight portion gamma-butyrolactons obtain epoxy resin solution B-1.Use ball mill that dispersion liquid A-1 is mixed with epoxy resin solution B-1, make paste composition C-1.The boiling point of gamma-butyrolacton is 204 ℃.Use mould to be coated with method this paste composition C-1 is coated on the aluminium base that thickness is 300 μ m, use baking oven, make it after 80 ℃ * 15 minutes dryings, under 175 ℃ * 1 hour condition, be cured, obtain the high dielectric composition of thickness 10 μ m.

Then, forming diameter by vapour deposition method on this high-k composition is the aluminium electrode of 11mm, use electric impedance analyzer HP 4284A and sample fixer HP 16451B (being Hewlett-Packard's system), with JIS K 6911 is benchmark, dielectric property under the 1MHz is measured, be the results are shown in table 1.The dielectric constant of high dielectric composition is 82, and dielectric loss angle tangent is 2.8%, and the static capacity of unit are is 7.3nF/cm ²Voidage is 9 volume %.

Embodiment 2

Produce paste composition C-1 similarly to Example 1.Then, further add 22.6 weight portion gamma-butyrolactons, make the quantity of solvent in the paste composition reach 15 weight %, produce paste composition C-2.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 1 based on the method for embodiment 1.The dielectric constant of high dielectric composition is 73, and dielectric loss angle tangent is 3.4%, and the static capacity of unit are is 4.3nF/cm ²Voidage is 12 volume %.

Embodiment 3～4

In paste composition C-1, further add gamma-butyrolacton, make the quantity of solvent in the paste composition reach 20,25 weight %, produce the different paste composition C-3～C-4 of quantity of solvent.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 1 based on the method for embodiment 1.Obtain voidage and be 20 volume % or below it, and dielectric constant is 50 or its above high dielectric composition.

Comparative example 1

In paste composition C-1, add gamma-butyrolacton, produce the paste composition D-1 that quantity of solvent in the paste composition accounts for 40 weight %.In addition,, produce the high dielectric composition, the evaluation result of dielectric property is shown in table 4 based on the method for embodiment 1.When the quantity of solvent that contains in the paste composition accounted for 40 weight % of total amount, voidage was 31 volume %, and dielectric constant is 41.

Embodiment 5

Use homogenizer with 323 weight portion barium titanates (Sakai chemistry (strain) system, BT-05, average grain diameter: 0.5 μ m), 0.2 weight portion dispersant (PVC ッ Network ケ ミ one (strain) system, BYK-W903), 18 weight portion gamma-butyrolactons are mixing, obtain dispersion liquid A-2.Use ball mill that dispersion liquid A-2 is mixed with epoxy resin solution B-1, produce paste composition C-5.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 1 based on the method for embodiment 1.Dielectric constant is 102, and dielectric loss angle tangent is 3.6%, and the static capacity of unit are is 11.3nF/cm ², voidage is 6 volume %.

Embodiment 6

Add gamma-butyrolacton in paste composition C-5, the quantity of solvent of producing in the paste composition is the paste composition C-6 of 15 weight %.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 1 based on the method for embodiment 1.Dielectric constant is 95, and dielectric loss angle tangent is 3.1%, and the static capacity of unit are is 8.4nF/cm ², voidage is 7 volume %.

Embodiment 7

Except solvent was the N-N-methyl-2-2-pyrrolidone N-, C-2 operated equally with paste composition, made paste composition, obtained paste composition C-7.The boiling point of N-N-methyl-2-2-pyrrolidone N-is 202 ℃.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 1 based on the method for embodiment 1.Dielectric constant is 58, and dielectric loss angle tangent is 4.6%, and the static capacity of unit are is 5.3nF/cm ², voidage is 26 volume %.

Embodiment 8

Except solvent was diacetate glycol ester, C-2 operated equally with paste composition, made paste composition, obtained paste composition C-8.The boiling point of diacetate glycol ester is 190 ℃.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 1 based on the method for embodiment 1.Dielectric constant is 64, and dielectric loss angle tangent is 4.8%, and the static capacity of unit are is 5.7nF/cm ², voidage is 21 volume %

Embodiment 9

Except solvent was ethyl carbitol, C-2 operated equally with paste composition, made paste composition, obtained paste composition C-9.The boiling point of ethyl carbitol is 202 ℃.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 2 based on the method for embodiment 1.Dielectric constant is 50, and dielectric loss angle tangent is 2.2%, and the static capacity of unit are is 4.4nF/cm ², voidage is 30 volume %.

Comparative example 2

Except solvent was morpholine, C-2 operated equally with paste composition, made paste composition, obtained paste composition D-2.The boiling point of morpholine is 128 ℃.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 4 based on the method for embodiment 1.Dielectric constant is 35, and dielectric loss angle tangent is 5.8%, and the static capacity of unit are is 2.6nF/cm ², electrical characteristics are poor.Voidage is 32 volume %

Comparative example 3

Except solvent was propylene glycol monomethyl ether, C-2 operated equally with paste composition, made paste composition, obtained paste composition D-3.The boiling point of propylene glycol monomethyl ether is 146 ℃.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 4 based on the method for embodiment 1.Dielectric constant is 46, and dielectric loss angle tangent is 4.7%, and the static capacity of unit are is 2.7nF/cm ², electrical characteristics are poor.Voidage is 35 volume %

Embodiment 10

0.5 μ m), 71 weight portion gamma-butyrolactons are mixing, obtain dispersion liquid A-3 use homogenizer with 494 weight portion barium titanates (Sakai chemistry (strain) system, BT-05, average grain diameter:.Use ball mill that dispersion liquid A-3 is mixed with epoxy resin solution B-1, produce paste composition C-10.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 2 based on the method for embodiment 1.Dielectric constant is 79, and dielectric loss angle tangent is 3.4%, and the static capacity of unit are is 5.8nF/cm ², voidage is 13 volume %.

Embodiment 11

0.5 μ m), 16 weight portion gamma-butyrolactons are mixing, obtain dispersion liquid A-4 use homogenizer with 185 weight portion barium titanates (Sakai chemistry (strain) system, BT-05, average grain diameter:.Use ball mill that dispersion liquid A-4 is mixed with epoxy resin solution B-1, produce paste composition C-11.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 2 based on the method for embodiment 1.Dielectric constant is 76, and dielectric loss angle tangent is 3.2%, and the static capacity of unit are is 8.4nF/cm ², voidage is 5 volume %.

Embodiment 12

(average grain diameter: 0.5 μ m) as beyond the high-k inorganic filler, paste composition C-12 is produced in operation similarly to Example 2 for eastern nation titanium (strain) system, SB05 except using barium titanate.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 2 based on the method for embodiment 1.Dielectric constant is 70, and dielectric loss angle tangent is 2.9%, and the static capacity of unit are is 6.2nF/cm ², voidage is 14 volume %.

Embodiment 13

(average grain diameter: 0.3 μ m) as beyond the high-k inorganic filler, paste composition C-13 is produced in operation similarly to Example 2 for Sakai chemistry (strain) system, ST-03 except using strontium titanates.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 2 based on the method for embodiment 1.Dielectric constant is 65, and dielectric loss angle tangent is 1.2%, and the static capacity of unit are is 3.8nF/cm ², voidage is 14 volume %.

Embodiment 14～16

Except using the resin shown in the table 2, curing agent, paste composition C-14～16 are produced in operation similarly to Example 2.Make the high dielectric composition, the evaluation result of dielectric property is shown in table 2.Obtain dielectric constant and be 50 or its above high dielectric composition.

Embodiment 17～18

Use as the polyimide resin of resin (east beautiful (strain) system, " セ ミ コ Off ァ ィ Application " SP341), (Sumitomo Chemical (strain) system 5003P), is produced paste composition C-17～18 to polyether sulfone.Make the high dielectric composition of forming shown in the table 3, estimate dielectric property.It is the results are shown in table 3.Obtain dielectric constant and be 50 or its above high dielectric composition.

Embodiment 19

Use homogenizer ice-cooled 0.5 μ m), 36 weight portion gamma-butyrolactons mix and disperseed 1 hour, obtain dispersion liquid A-5 down with 323 weight portion barium titanate fillers (Sakai chemistry (strain) system, BT-05, average grain diameter:.With 12.8 weight portion epoxy resin (Japanese chemical drug (strain) system, EPPN502H), 7.8 weight portion phenol novolac resins (big Japanese ィ Application キ industry (strain) system, TD-2131), ((strain) system is learned in northern Xinghua to 0.2 weight portion curing accelerator, triphenylphosphine), 24.8 the weight portion gamma-butyrolacton mixes, and obtains epoxy resin solution B-2.Use ball mill that dispersion liquid A-5 is mixed with epoxy resin solution B-2, produce paste composition C-19.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 3 based on the method for embodiment 1.Dielectric constant is 73, and dielectric loss angle tangent is 3.4%, and the static capacity of unit are is 4.3nF/cm ², voidage is 12 volume %.

Embodiment 20

Use homogenizer with 323 weight portion barium titanates (Sakai chemistry (strain) system, BT-05,0.5 μ m), 0.2 weight portion dispersant (the copolymer that contains acid group average grain diameter: with phosphate skeleton, PVC ッ Network ケ ミ one (strain) system, BYK-W9010), 36 weight portion gamma-butyrolactons are mixing, obtain dispersion liquid A-6.Use ball mill that dispersion liquid A-6 is mixed with epoxy resin solution B-2, make paste composition C-20.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 3 based on the method for embodiment 1.Dielectric constant is 95, and dielectric loss angle tangent is 3.1%, and the static capacity of unit are is 8.4nF/cm ², voidage is 7 volume %.

Embodiment 21

Mix 15.3 weight portion epoxy resin (Japanese chemical drug (strain) system, NC3000), 5.3 weight portion phenol novolac resins (Japanese chemical drug (strain) system, ((strain) system is learned in northern Xinghua for " カ ャ Ha one De " TPM (newname: " カ ャ Ha one De " KTG-105)), 0.2 weight portion curing accelerator, triphenylphosphine), 24.7 the weight portion gamma-butyrolacton obtains epoxy resin solution B-3.Use ball mill that dispersion liquid A-2 is mixed with epoxy resin solution B-3, produce paste composition C-21.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 3 based on the method for embodiment 1.Dielectric constant is 76, and dielectric loss angle tangent is 2.8%, and the static capacity of unit are is 5.6nF/cm ², voidage is 14 volume %.

Embodiment 22

Use homogenizer with 62.3 weight portion barium titanates (Sakai chemistry (strain) system, BT-05, average grain diameter 0.5 μ m), 21.9 weight portion barium titanate (TPL, Inc. society's system, average grain diameter 0.059 μ m), 15 weight portion gamma-butyrolactons, 0.8 weight portion dispersant (the copolymer that contains acid group HPB-1000: with phosphate skeleton, PVC ッ Network ケ ミ one ジ ャ パ Application (strain) system, BYK-W9010) mixing, obtain dispersion liquid A-7.With 2.2 weight portion epoxy resin (Japanese chemical drug (strain) system, EPPN502H), 1.4 weight portion phenol novolac resins (big Japanese ィ Application キ industry (strain) system, TD-2131), ((strain) system is learned in northern Xinghua to 0.04 weight portion curing accelerator, triphenylphosphine), 7.1 the weight portion gamma-butyrolacton mixes, and obtains epoxy resin solution B-4.Use ball mill that dispersion liquid A-7 is mixed with epoxy resin solution B-4, produce paste composition C-22.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 6 based on the method for embodiment 1.Dielectric constant is 123, and dielectric loss angle tangent is 3.1%, and the static capacity of unit are is 10.9nF/cm ², voidage is 4 volume %.

Embodiment 23

With 2.6 weight portion epoxy resin (Japanese chemical drug (strain) system, NC-3000), 0.9 weight portion phenol novolac resin (Japanese chemical drug (strain) system, ((strain) system is learned in northern Xinghua for " カ ャ Ha one De " TPM (newname: " カ ャ Ha one De " KTG-105)), 0.04 weight portion curing accelerator, triphenylphosphine), 7.1 the weight portion gamma-butyrolacton mixes, and obtains epoxy resin solution B-5.Use ball mill that dispersion liquid A-7 is mixed with epoxy resin solution B-5, produce paste composition C-23.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 6 based on the method for embodiment 1.Dielectric constant is 121, and dielectric loss angle tangent is 2.6%, and the static capacity of unit are is 10.7nF/em ², voidage is 4 volume %.

Embodiment 24

Except using diacetate glycol ester as the solvent, paste composition C-24 is produced in operation similarly to Example 23.The boiling point of diacetate glycol ester is 190 ℃.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 6 based on the method for embodiment 1.Dielectric constant is 95, and dielectric loss angle tangent is 3.1%, and the static capacity of unit are is 8.4nF/cm ², voidage is 8 volume %.

Embodiment 25

Except using diethyl malonate as the solvent, paste composition C-25 is produced in operation similarly to Example 23.The boiling point of diethyl malonate is 199 ℃.In addition,, make the high dielectric composition, estimate dielectric property based on the method for embodiment 1.Dielectric constant is 85, and dielectric loss angle tangent is 2.7%, and the static capacity of unit are is 7.5nF/cm ², voidage is 9 volume %.

Embodiment 26

Except using ethyl carbitol as the solvent, paste composition C-26 is produced in operation similarly to Example 23.The boiling point of ethyl carbitol is 202 ℃.In addition,, make the high dielectric composition, estimate dielectric property based on the method for embodiment 1.Dielectric constant is 99, and dielectric loss angle tangent is 2.9%, and the static capacity of unit are is 8.8nF/cm ², voidage is 7 volume %.

Embodiment 27

Except using the 4-methyl cyclohexanone as the solvent, paste composition C-27 is produced in operation similarly to Example 23.The boiling point of 4-methyl cyclohexanone is 169 ℃.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 6 based on the method for embodiment 1.Dielectric constant is 79, and dielectric loss angle tangent is 2.1%, and the static capacity of unit are is 7.0nF/cm ², voidage is 12 volume %.

Embodiment 28

Except using different fluorine that ketone as the solvent, paste composition C-28 is produced in operation similarly to Example 23.Your boiling point of ketone of different fluorine is 215 ℃.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 6 based on the method for embodiment 1.Dielectric constant is 76, and dielectric loss angle tangent is 2.2%, and the static capacity of unit are is 6.7nF/cm ², voidage is 11 volume %.

Embodiment 29

Except using diethylformamide as the solvent, paste composition C-29 is produced in operation similarly to Example 23.The boiling point of diethylformamide is 177 ℃.In addition,, make the high dielectric composition, the evaluation result of dielectric property is shown in table 6 based on the method for embodiment 1.Dielectric constant is 70, and dielectric loss angle tangent is 2.3%, and the static capacity of unit are is 6.2nF/cm ², voidage is 15 volume %.

Embodiment 30

Except using dimethylacetylamide as the solvent, paste composition C-30 is produced in operation similarly to Example 23.The boiling point of dimethylacetylamide is 165 ℃.In addition,, make the high dielectric composition, estimate dielectric property based on the method for embodiment 1.Dielectric constant is 79, and dielectric loss angle tangent is 2.3%, and the static capacity of unit are is 7.0nF/cm ², voidage is 11 volume %.

Synthesis example 1; Dispersion liquid X-1

Use homogenizer with 5328 weight portion barium titanate fillers (Sakai chemical industry (strain) system, BT-05, average grain diameter 0.5 μ m), 1872 weight portion barium titanate filler (TPL, Inc. society's system, average grain diameter 0.059 μ m), 928 weight portion gamma-butyrolactons, 72 weight portion dispersants (the copolymer that contains acid group HPB-1000: with phosphate skeleton, PVC ッ Network ケ ミ one ジ ャ パ Application (strain) system BYK-W9010) was disperseed 1 hour in ice-cooled the mixing down, obtained dispersion liquid X-1.

Synthesis example 2; Dispersion liquid X-2

Use homogenizer with 5328 weight portion barium titanate fillers (Sakai chemical industry (strain) system, BT-05,0.5 μ m), 1872 weight portion barium titanate filler (Cabot Corp. societies average grain diameter:, K-Plus16, average grain diameter 0.06 μ m), 928 weight portion gamma-butyrolactons, 72 weight portion dispersants (the copolymer that contains acid group with phosphate skeleton, PVC ッ Network ケ ミ one ジ ャ パ Application (strain) system BYK-W9010) was disperseed 1 hour in ice-cooled the mixing down, obtained dispersion liquid X-2.

Synthesis example 3; Dispersion liquid X-3

Use homogenizer with 5328 weight portion barium titanate fillers (Sakai chemical industry (strain) system, BT-02,0.18 μ m), 1872 weight portion barium titanate filler (TPL average grain diameter:, Inc. make, average grain diameter 0.059 μ m), 928 weight portion gamma-butyrolactons, 72 weight portion dispersants (the copolymer that contains acid group HPB-1000: with phosphate skeleton, PVC ッ Network ケ ミ one ジ ャ パ Application (strain) system BYK-W9010) was disperseed 1 hour in ice-cooled the mixing down, obtained dispersion liquid X-3.

Synthesis example 4; Dispersion liquid X-4

Use homogenizer with 5328 weight portion barium titanate fillers (Sakai chemical industry (strain) system, BT-03,0.28 μ m), 1872 weight portion barium titanate filler (TPL average grain diameter:, Inc. make, average grain diameter 0.059 μ m), 928 weight portion gamma-butyrolactons, 72 weight portion dispersants (the copolymer that contains acid group HPB-1000: with phosphate skeleton, PVC ッ Network ケ ミ one ジ ャ パ Application (strain) system BYK-W9010) was disperseed 1 hour in ice-cooled the mixing down, obtained dispersion liquid X-4.

Synthesis example 5; Dispersion liquid X-5

Use homogenizer with 5328 weight portion barium titanate fillers (upright altogether マ テ リ ァ Le (strain) system, BT-HP3,1.2 μ m), 1872 weight portion barium titanate filler (TPL average grain diameter:, Inc. make, average grain diameter 0.059 μ m), 928 weight portion gamma-butyrolactons, 72 weight portion dispersants (the copolymer that contains acid group HPB-1000: with phosphate skeleton, PVC ッ Network ケ ミ one ジ ャ パ Application (strain) system BYK-W9010) was disperseed 1 hour in ice-cooled the mixing down, obtained dispersion liquid X-5.

Synthesis example 6; Dispersion liquid X-6

Use homogenizer with 5328 weight portion barium titanate fillers (upright altogether マ テ リ ァ Le (strain) system, BT-SA, 2.1 μ m), 1872 weight portion barium titanate filler (TPL average grain diameter:, Inc. make, average grain diameter 0.059 μ m), 928 weight portion gamma-butyrolactons, 72 weight portion dispersants (the copolymer that contains acid group HPB-1000: with phosphate skeleton, PVC ッ Network ケ ミ one ジ ャ パ Application (strain) system BYK-W9010) was disperseed 1 hour in ice-cooled the mixing down, obtained dispersion liquid X-6.

Synthesis example 7; Dispersion liquid X-7

Use homogenizer with 6067 weight portion barium titanate fillers (Sakai chemical industry (strain) system, BT-05,0.5 μ m), 1613 weight portion strontium titanates filler (TPL average grain diameter:, Inc. make, average grain diameter 0.045 μ m), 1523 weight portion gamma-butyrolactons, 77 weight portion dispersants (the copolymer that contains acid group HPS-2000: with phosphate skeleton, PVC ッ Network ケ ミ one ジ ャ パ Application (strain) system BYK-W9010) was disperseed 1 hour in ice-cooled the mixing down, obtained dispersion liquid X-7.

Synthesis example 8; Dispersion liquid X-8

Use homogenizer with 5261 weight portion barium titanate fillers (Sakai chemical industry (strain) system, BT-05, average grain diameter 0.5 μ m), 2419 parts by weight of titanium oxide fillers (eastern nation titanium (strain) system, HT0514,0.2 μ m), 1523 weight portion gamma-butyrolactons, 77 weight portion dispersants (the copolymer that contains acid group average grain diameter: with phosphate skeleton, PVC ッ Network ケ ミ one ジ ャ パ Application (strain) system BYK-W9010) was disperseed 1 hour in ice-cooled the mixing down, obtained dispersion liquid X-8.

Synthesis example 9; Dispersion liquid X-9

Use homogenizer with the plumbous class filler of 6695 weight portions (Ferro society system, Y5V183U, 0.9 μ m), 1145 weight portion barium titanate filler (TPL average grain diameter:, Inc. make, average grain diameter 0.059 μ m), 1722 weight portion gamma-butyrolactons, 78 weight portion dispersants (the copolymer that contains acid group HPB-1000: with phosphate skeleton, PVC ッ Network ケ ミ one ジ ャ パ Application (strain) system BYK-W9010) was disperseed 1 hour in ice-cooled the mixing down, obtained dispersion liquid X-9.

Synthesis example 10; Dispersion liquid X-10

Use homogenizer with 7200 weight portion barium titanate fillers (Sakai chemical industry (strain) system, BT-05,0.5 μ m), 928 weight portion gamma-butyrolactons, 72 weight portion dispersant (copolymers average grain diameter: with phosphoric acid ester acid group, PVC ッ Network ケ ミ one ジ ャ パ Application (strain) system, BYK-W9010) disperseed 1 hour in ice-cooled the mixing down, obtain dispersion liquid X-10.

Synthesis example 11; Dispersion liquid X-11

Use homogenizer with 5328 weight portion barium titanate fillers (upright altogether マ テ リ ァ Le (strain) system, BTHP-8YF, 7 μ m), 1872 weight portion barium titanate fillers (Sakai chemical industry (strain) system average grain diameter:, BT-05,0.5 μ m), 928 weight portion gamma-butyrolactons, 72 weight portion dispersants (the copolymer that contains acid group average grain diameter: with phosphate skeleton, PVC ッ Network ケ ミ one ジ ャ パ Application (strain) system BYK-W9010) was disperseed 1 hour in ice-cooled the mixing down, obtained dispersion liquid X-11.

Synthesis example 12; Dispersion liquid X-12

Use ball mill with barium titanate filler (upright altogether マ テ リ ァ Le (strain) system, BT-SA, average grain diameter: after 2.1 μ m) being distributed in the acrylic resin binder, use spray dryer to make the primary particle aggegation be solidified into offspring, this offspring is carried out granulation.With its in atmosphere, 1200 ℃ burn till 6 hours after, pulverize with mortar, carry out classification by 500 orders and 300 purposes sieve then, obtain the barium titanate filler A of average grain diameter 40 μ m.Use a dynamic scattering formula particle size distribution analyzer ((strain) rise abruptly make a made LB-500) to average the mensuration of particle diameter.Use homogenizer with this barium titanate filler of 5328 weight portions A, 1872 weight portion barium titanate filler B (upright altogether マ テ リ ァ Le (strain) system, BT-SA, 2.1 μ m), 928 weight portion gamma-butyrolactons, 72 weight portion dispersants (copolymer that contains acid group with phosphate skeleton, PVC ッ Network ケ ミ one ジ ャ パ Application average grain diameter:

(strain) system BYK-W9010) was disperseed 1 hour in ice-cooled the mixing down, obtained dispersion liquid X-12.

Synthesis example 13; Dispersion liquid X-13

Except using 1000 orders and 600 purposes sieve to carry out the classification, operate equally with the barium titanate filler A of synthesis example 12, obtain the barium titanate filler C of average grain diameter 20 μ m.Use homogenizer with this barium titanate filler of 5328 weight portions C, 1872 weight portion barium titanate filler B (upright altogether マ テ リ ァ Le (strain) system, BT-SA, 2.1 μ m), 928 weight portion gamma-butyrolactons, 72 weight portion dispersants (the copolymer that contains acid group average grain diameter: with phosphate skeleton, PVC ッ Network ケ ミ one ジ ャ パ Application (strain) system, BYK-W9010) disperseed 1 hour in ice-cooled the mixing down, obtain dispersion liquid X-13.

Synthesis example 14; Epoxy resin solution Y-1

Mix 400 weight portion epoxy resin (Japanese chemical drug (strain) system, EPPN-502H), (big Japanese ィ Application キ industry (strain) system TD-2131), 1000 weight portion gamma-butyrolactons, obtains resin solution Y-1 to 400 weight portion phenol novolac resins.

Synthesis example 15; Epoxy resin solution Y-2

Mix 600 weight portion epoxy resin (Japanese chemical drug (strain) system, NC-3000), 200 weight portion phenol novolac resins (Japanese chemical drug (strain) system, ((strain) system is learned in northern Xinghua for " カ ャ Ha one De " TPM (newname: " カ ャ Ha one De " KTG-105)), 8 weight portion curing accelerators, triphenylphosphine), 1000 weight portion gamma-butyrolactons obtain resin solution Y-2.

Embodiment 31

In possessing the container of blender, add 82 weight portion dispersion liquid X-1, add 18 parts by weight resin solution Y-1 slowly, use Let Down method to mix, then, further stirred 1 hour, obtain paste composition with ball mill.The content of the inorganic filler when at this moment, the total amount of establishing inorganic filler and resin is 100 volume % is about 61 volume %.

Then, use spin-coating method that this paste composition is coated on aluminium base and the copper base, use baking oven, solidified 1 hour at 175 ℃ then, obtain dielectric composition 120 ℃ of dryings 10 minutes.Use the stress determination device Flexus of Tencor society system, the STRESS VARIATION that the temperature of the dielectric composition that forms on these 2 kinds of substrates causes is measured, calculate the coefficient of linear expansion of dielectric composition from this rate of change, the result is good, be 18ppm/ ℃, with copper (17ppm/ ℃) basically identical.

And then, on the surface of the dielectric composition on the aluminium base, form the aluminium electrode by vapour deposition method, with the aluminium of itself and substrate as electrode, use electric impedance analyzer (Hewlett-Packard's system, HP4284A HP16451B), is a benchmark with JIS K6911, measure its dielectric property under 1MHz, dielectric constant is 55 as a result, and dielectric loss angle tangent is 3.3%, and the static capacity of unit are is 4.9nF/cm ²

In addition, dielectric composition on the copper base is carried out Pressure Cooker Test (PCT test, 100%RH, 121 ℃, 2 atmospheric pressure are after 100 hours), the result does not find any unusual with electron microscope, utilize in the test (JIS K5400) of gridiron pattern adhesive tape method, evaluation score is 10 minutes, and is good.

In addition, in arbitrary mensuration of coefficient of linear expansion, dielectric property, PCT test, be that 3 levels of 5,10,20 μ m are estimated all, but do not find the difference that thickness causes, the result when therefore in table 9, having summed up 10 μ m with the thickness of dielectric composition.

Embodiment 32

In possessing the container of blender, add 86 weight portion dispersion liquid X-1, add 11 parts by weight resin solution Y-1 and 3 weight portion gamma-butyrolactons slowly, use Let Down method to mix, and then stirred 1 hour, obtain paste composition with ball mill.The content of the inorganic filler when at this moment, the total amount of establishing inorganic filler and resin is 100 volume % is about 72 volume %.

Use the paste composition obtain like this, according to obtaining dielectric composition, the measurement result of coefficient of linear expansion, dielectric property, PCT test is shown in table 9 with the same method of embodiment 31.

Embodiment 33

In possessing the container of blender, add 88 weight portion dispersion liquid X-1, add 7 parts by weight resin solution Y-1 and 5 weight portion gamma-butyrolactons slowly, use Let Down method to mix, then, further stirred 1 hour, obtain paste composition with ball mill.The content of the inorganic filler when at this moment, the total amount of establishing inorganic filler and resin is 100 volume % is about 79 volume %.Use the paste composition that obtains like this, obtain dielectric composition according to embodiment 31 same methods, the measurement result that coefficient of linear expansion, dielectric property, PCT are tested is shown in table 9.

Embodiment 34

In possessing the container of blender, add 89 weight portion dispersion liquid X-1, add 4 parts by weight resin solution Y-1 and 7 weight portion gamma-butyrolactons slowly, use Let Down method to mix, then, further stirred 1 hour, obtain paste composition with ball mill.The content of the inorganic filler when at this moment, the total amount of establishing inorganic filler and resin is 100 volume % is about 86 volume %.Use the paste composition that obtains like this, obtain dielectric composition according to embodiment 31 same methods, the measurement result that coefficient of linear expansion, dielectric property, PCT are tested is shown in table 9.

Embodiment 35

In possessing the container of blender, add 90 weight portion dispersion liquid X-1, add 2 parts by weight resin solution Y-1 and 8 weight portion gamma-butyrolactons slowly, use Let Down method to mix, then, further stirred 1 hour, obtain paste composition with ball mill.The content of the inorganic filler when at this moment, the total amount of establishing inorganic filler and resin is 100 volume % is about 91 volume %.Use the paste composition that obtains like this, obtain dielectric composition according to embodiment 31 same methods, the measurement result that coefficient of linear expansion, dielectric property, PCT are tested is shown in table 9.

Embodiment 36

In possessing the container of blender, add 91 weight portion dispersion liquid X-1, add 1 parts by weight resin solution Y-1 and 8 weight portion gamma-butyrolactons slowly, use Let Down method to mix, then, further stirred 1 hour, obtain paste composition with ball mill.The content of the inorganic filler when at this moment, the total amount of establishing inorganic filler and resin is 100 volume % is about 93 volume %.Use the paste composition that obtains like this, obtain dielectric composition according to embodiment 31 same methods, the measurement result that coefficient of linear expansion, dielectric property, PCT are tested is shown in table 9.

Embodiment 37～43

In possessing the container of blender, add the dispersion liquid shown in the 88 weight portion tables 5, slowly add resin solution shown in the 7 weight portion tables 5 and 5 weight portion gamma-butyrolactons, use Let Down method to mix, then, further stirred 1 hour, obtain paste composition with ball mill.The content of the inorganic filler when at this moment, the total amount of establishing inorganic filler and resin is 100 volume % is about 79 volume %.Use the paste composition that obtains like this, obtain dielectric composition according to embodiment 31 same methods, the measurement result of coefficient of linear expansion, dielectric property, PCT test is represented in table 9, table 10.

Embodiment 44

In possessing the container of blender, add 93 weight portion dispersion liquid X-7, add 7 parts by weight resin solution Y-1 slowly, use Let Down method to mix, then, further stirred 1 hour, obtain paste composition with ball mill.The content of the inorganic filler when at this moment, the total amount of inorganic filler and resin being 100 volume % is adjusted into about 79 volume %.Use the paste composition that obtains like this, obtain dielectric composition according to embodiment 31 same methods, the measurement result that coefficient of linear expansion, dielectric property, PCT are tested is shown in table 10.

Embodiment 45

In possessing the container of blender, add 93 weight portion dispersion liquid X-8, add 7 parts by weight resin solution Y-1 slowly, use Let Down method to mix, then, further stirred 1 hour, obtain paste composition with ball mill.The content of the inorganic filler when at this moment, the total amount of inorganic filler and resin being 100 volume % is adjusted into about 81 volume %.Use the paste composition that obtains like this, obtain dielectric composition according to embodiment 31 same methods, the measurement result that coefficient of linear expansion, dielectric property, PCT are tested is shown in table 10.

Embodiment 46

In possessing the container of blender, add 93 weight portion dispersion liquid X-9, add 7 parts by weight resin solution Y-1 slowly, use Let Down method to mix, then, further stirred 1 hour, obtain paste composition with ball mill.The content of the inorganic filler when at this moment, the total amount of inorganic filler and resin being 100 volume % is adjusted into about 86 volume %.Use the paste composition that obtains like this, obtain dielectric composition according to embodiment 31 same methods, the measurement result that coefficient of linear expansion, dielectric property, PCT are tested is shown in table 10.

Comparative example 4

Except using the epoxy resin solution of synthesis example 14, do not use beyond the inorganic filler dispersion liquid, operate equally with embodiment 31, obtain dielectric composition, the measurement result that coefficient of linear expansion, dielectric property, PCT are tested is shown in table 10.

Comparative example 5

In possessing the container of blender, add 88 weight portion dispersion liquid X-10, add 7 parts by weight resin solution Y-1 and 5 weight portion gamma-butyrolactons slowly, use Let Down method to mix, then, further stirred 1 hour, obtain paste composition with ball mill.The content of the inorganic filler when at this moment, the total amount of establishing inorganic filler and resin is 100 volume % is about 79 volume %.Use the paste composition that obtains like this, operate equally with embodiment 31, obtain dielectric composition, the measurement result that coefficient of linear expansion, dielectric property, PCT are tested is shown in table 10.

Comparative example 6

In possessing the container of blender, add 88 weight portion dispersion liquid X-11, add 7 parts by weight resin solution Y-1 and 5 weight portion gamma-butyrolactons slowly, use Let Down method to mix, then, further stirred 1 hour, obtain paste composition with ball mill.This paste composition causes sedimentation because of placement easily.The content of the inorganic filler when at this moment, the total amount of establishing inorganic filler and resin is 100 volume % is about 79 volume %.Use the paste composition that obtains like this, operate equally, obtain dielectric composition, attempt carrying out the mensuration of dielectric property, but the measured value instability can not be measured with embodiment 31.

Comparative example 7

In possessing the container of blender, add 88 weight portion dispersion liquid X-12, add 7 parts by weight resin solution Y-1 and 5 weight portion gamma-butyrolactons slowly, use Let Down method to mix, then, further stirred 1 hour, obtain paste composition with ball mill.This paste composition causes sedimentation because of placement easily.The content of the inorganic filler when at this moment, the total amount of establishing inorganic filler and resin is 100 volume % is about 79 volume %.Use the paste composition that obtains like this, operate equally, obtain dielectric composition, attempt carrying out the mensuration of dielectric property, but the measured value instability can not be measured with embodiment 31.

Comparative example 8

In possessing the container of blender, add 8893 weight portion dispersion liquid X-13, add 7 parts by weight resin solution Y-1 and 5 weight portion gamma-butyrolactons slowly, use Let Down method to mix, then, further stirred 1 hour, obtain paste composition with ball mill.This paste composition causes sedimentation because of placement easily.The content of the inorganic filler when at this moment, the total amount of establishing inorganic filler and resin is 100 volume % is about 79 volume %.Use the paste composition that obtains like this, operate equally, obtain dielectric composition, attempt carrying out the mensuration of dielectric property, but the measured value instability can not be measured with embodiment 31.

Comparative example 9

Except barium titanate filler (Sakai chemical industry (strain) system with big particle diameter filler, BT-05, average grain diameter: 0.5 μ m) become barium titanate filler (TPL, Inc. make, HPB-1000: average grain diameter 0.059 μ m), barium titanate filler (TPL with the small particle diameter filler, Inc. make HPB-1000: average grain diameter 0.059 μ m) become strontium titanates filler (TPL, Inc. system, HPS-2000: average grain diameter 0.045 μ m) in addition, operate equally with synthesis example 3, attempt making dispersion liquid, but filler generation aggegation, the dispersion liquid instability fails to obtain paste composition.

The industry utilizability

Paste composition of the present invention and dielectric composition are applicable to capacitor or have purposes such as interlayer dielectic that the circuit material of capacitor function uses or light wiring material.

Table 1

	Paste composition							Dielectric property (1MHz)				Membrane property
													Embodiment	Inorganic filler	Resin	Curing agent	Solvent	Additive	Gu form the content (weight %) of inorganic filler in dividing	Quantity of solvent in the paste composition total amount (weight %)	Thickness (μ m)	Dielectric constant	Static capacity (nF/cm 2)	Dielectric loss angle tangent (%)	Voidage (volume %)
1	Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Gamma-butyrolacton	Triphenylphosphine	94	10	10	82	7.3	2.8	9
													2	Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Gamma-butyrolacton	Triphenylphosphine	94	15	15	73	4.3	3.4	12
3	Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Gamma-butyrolacton	Triphenylphosphine	94	20	10	65	5.8	3.0	14
													4	Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Gamma-butyrolacton	Triphenylphosphine	94	25	8	58	6.4	3.2	20
5	Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Gamma-butyrolacton	Triphenylphosphine	94	10	8	102	11.3	3.6	6
													BYK-W903
					6									Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Gamma-butyrolacton	Triphenylphosphine	94	15	10	95	8.4	3.1	7
BYK-W903
	7	Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin		N-methyl-2-pyrrolidones	Triphenylphosphine	94	15	10	58	5.3	4.6					26
8					Barium titanate Sakai chemistry BT-05									Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Diacetate glycol ester	Triphenylphosphine		94	15	10	64	5.7	4.8	21

Table 2

Paste composition

Dielectric property (1MHz)

Membrane property

Embodiment

Inorganic filler

Resin

Curing agent

Solvent

Additive

Gu form the content (weight %) of inorganic filler in dividing

Quantity of solvent in the paste composition total amount (weight %)

Thickness (μ m)

Dielectric constant

Static capacity (nF/cm 2)

Dielectric loss angle tangent (%)

Voidage (volume %)

9	Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Ethyl carbitol	Triphenylphosphine	94	15	10	50	4.4	2.2	30
													10	Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Gamma-butyrolacton	Triphenylphosphine	96	15	12	79	5.8	3.4	13
11	Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Gamma-butyrolacton	Triphenylphosphine	90	15	8	76	8.4	3.2	5
													12	The barium titanate east titanium SB05 of nation	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Gamma-butyrolacton	Triphenylphosphine	94	15	10	70	6.2	2.9	14
13	Strontium titanates Sakai chemistry ST-03	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Gamma-butyrolacton	Triphenylphosphine	94	15	15	65	3.8	1.2	14
													14	Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug NC3000	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Gamma-butyrolacton	Triphenylphosphine	94	15	15	71	4.2	2.7	16
15	Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug NC3000	Phenol novolac resin Japan chemical drug カ ャ Ha one De TPM	Gamma-butyrolacton	Triphenylphosphine	94	15	12	76	5.6	2.8	14
													16	Barium titanate Sakai chemistry BT-05	The big Japanese ィ Application キ HP7200 of epoxy resin	The big Japanese ィ Application キ VH4150 of phenol novolac resin	Gamma-butyrolacton	Triphenylphosphine	94	15	10	69	6.1	3.0	16

Table 3

	Paste composition							Dielectric property (1MHz)				Membrane property
													Embodiment	Inorganic filler	Resin	Curing agent	Solvent	Additive	Gu form the content (weight %) of inorganic filler in dividing	Quantity of solvent in the paste composition total amount (weight %)	Thickness (μ m)	Dielectric constant	Static capacity (nF/cm 2)	Dielectric loss angle tangent (%)	Voidage (volume %)
17	Barium titanate Sakai chemistry BT-05	The beautiful セ ミ コ Off ァ ィ Application-SP341 in polyimide resin east	-	Gamma-butyrolacton	-	94	15	10	68	6.0	0.7	17
													18	Barium titanate Sakai chemistry BT-05	Polyether sulfone Sumitomo Chemical 5003P	-	Gamma-butyrolacton	-	94	15	8	65	7.2	0.5	17
19	Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Gamma-butyrolacton	Triphenylphosphine	94	15	15	73	4.3	3.4	12
													20	The barium titanate east titanium SB05 of nation	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Gamma-butyrolacton	Triphenylphosphine	94	15	10	95	8.4	3.1	7
BYK-W90 10
	21	Strontium titanates Sakai chemistry ST-03	Epoxy resin Japan chemical drug NC3000	Phenol novolac resin Japan chemical drug カ ャ Ha one De TPM	Gamma-butyrolacton	Triphenylphosphine	94	15	12	76	5.6	2.8						14

Table 4

Paste composition

Dielectric property (1MHz)

Membrane property

Comparative example

Inorganic filler

Resin

Curing agent

Solvent

Additive

Gu form the content (weight %) of inorganic filler in dividing

Quantity of solvent in the paste composition total amount (weight %)

Thickness (μ m)

Dielectric constant

Static capacity (nF/cm 2 )

Dielectric loss angle tangent (%)

Voidage (volume %)

1	Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Gamma-butyrolacton	Triphenylphosphine	94	40	15	41	2.4	4.9	31
													2	Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Morpholine	Triphenylphosphine	94	15	12	35	2.6	5.8	32
3	Barium titanate Sakai chemistry BT-05	Epoxy resin Japan chemical drug EPPN502H	The big Japanese ィ Application キ TD2131 of phenol novolac resin	Propylene glycol monomethyl ether	Triphenylphosphine	94	15	15	46	2.7	4.7	35

Table 5

Paste composition

Inorganic filler

Resin

Curing agent

Solvent

Additive

Gu form the content (weight %) of inorganic filler in dividing

Quantity of solvent in the paste composition total amount (weight %)

A

B

Embodiment 22

Barium titanate Sakai chemistry BT-05

Barium titanate TPL.IncHPB-1000

Epoxy resin Japan chemical drug EPPN502H

The big Japanese ィ Application キ TD2131 of phenol novolac resin

Gamma-butyrolacton

Triphenylphosphine

96

20

BYK-W9010

Embodiment 23

Barium titanate Sakai chemistry BT-05

Barium titanate TPL.IncHPB-1000

Epoxy resin Japan chemical drug NC3000

Phenol novolac resin Japan chemical drug カ ャ Ha one De TPM

Gamma-butyrolacton

Triphenylphosphine

96

20

BYK-W9010

Embodiment 24

Barium titanate Sakai chemistry BT-05

Barium titanate TPL.IncHPB-1000

Epoxy resin Japan chemical drug NC3000

Phenol novolac resin Japan chemical drug カ ャ Ha one De TPM

Diacetate glycol ester

Triphenylphosphine

96

20

BYK-W9010

Embodiment 25

Barium titanate Sakai chemistry BT-05

Barium titanate TPL.IncHPB-1000

Epoxy resin Japan chemical drug NC3000

Phenol novolac resin Japan chemical drug カ ャ Ha one De TPM

Diethyl malonate

Triphenylphosphine

96

20

BYK-W9010

Embodiment 26

Barium titanate Sakai chemistry BT-05

Barium titanate TPL.IncHPB-1000

Epoxy resin Japan chemical drug NC3000

Phenol novolac resin Japan chemical drug カ ャ Ha one De TPM

Ethyl carbitol

Triphenylphosphine

96

20

BYK-W9010

Embodiment 27

Barium titanate Sakai chemistry BT-05

Barium titanate TPL.IncHPB-1000

Epoxy resin Japan chemical drug NC3000

Phenol novolac resin Japan chemical drug カ ャ Ha one De TPM

The 4-methyl cyclohexanone

Triphenylphosphine

96

20

BYK-W9010

Embodiment 28

Barium titanate Sakai chemistry BT-05

Barium titanate TPL.IncHPB-1000

Epoxy resin Japan chemical drug NC3000

Phenol novolac resin Japan chemical drug カ ャ Ha one De TPM

Different fluorine that ketone

Triphenylphosphine

96

20

BYK-W9010

Embodiment 29

Barium titanate Sakai chemistry BT-05

Barium titanate TPL.IncHPB-1000

Epoxy resin Japan chemical drug NC3000

Phenol novolac resin Japan chemical drug カ ャ Ha one De TPM

Diethylformamide

Triphenylphosphine

96

20

BYK-W9010

Embodiment 30

Barium titanate Sakai chemistry BT-05

Barium titanate TPL.IncHPB-1000

Epoxy resin Japan chemical drug NC3000

Phenol novolac resin Japan chemical drug カ ャ Ha one De TPM

Dimethylacetylamide

Triphenylphosphine

96

20

BYK-W9010

Table 6

	Dielectric property (1MHz)				Membrane property
							Thickness (μ m)	Dielectric constant	Static capacity (nF/cm 2)	Dielectric loss angle tangent (%)	Voidage (volume %)
Embodiment 22	10	123	10.9	3.1	4
						Embodiment 23	10	121	10.7	2.6	4
Embodiment 24	10	95	8.4	3.1	8
						Embodiment 25	10	85	7.5	2.7	9
Embodiment 26	10	99	8.8	2.9	7
						Embodiment 27	10	79	7.0	2.1	12
Embodiment 28	10	76	6.7	2.2	11
						Embodiment 29	10	70	6.2	2.3	15
Embodiment 30	10	79	7.0	2.3	11

Table 7

Paste composition

Dispersion liquid

Inorganic filler

Resin solution

The ratio of inorganic filler/resin

Dispersion stabilization

Form

Average grain diameter (μ m)

Form

Average grain diameter (μ m)

Maximum/minimum (ratio)

Epoxy resin

Volume ratio

Embodiment 31

?X-1

Barium titanate

0.5

Barium titanate

0.059

8.5

Y-1

61/39

Stable

Embodiment 32

?X-1

Barium titanate

0.5

Barium titanate

0.059

8.5

Y-1

72/28

Stable

Embodiment 33

?X-1

Barium titanate

0.5

Barium titanate

0.059

8.5

Y-1

79/21

Stable

Embodiment 34

?X-1

Barium titanate

0.5

Barium titanate

0.059

8.5

Y-1

86/14

Stable

Embodiment 35

?X-1

Barium titanate

0.5

Barium titanate

0.059

8.5

Y-1

91/9

Stable

Embodiment 36

?X-1

Barium titanate

0.5

Barium titanate

0.059

8.5

Y-1

93/7

Stable

Embodiment 37

?X-1

Barium titanate

0.5

Barium titanate

0.059

8.5

Y-2

79/21

Stable

Embodiment 38

?X-2

Barium titanate

0.5

Barium titanate

0.060

8.3

Y-2

79/21

Stable

Embodiment 39

?X-3

Barium titanate

0.18

Barium titanate

0.059

3.1

Y-1

79/21

Stable

Embodiment 40

?X-4

Barium titanate

0.28

Barium titanate

0.059

4.7

Y-1

79/21

Stable

Embodiment 41

?X-5

Barium titanate

1.2

Barium titanate

0.059

20.3

Y-1

79/21

Unstable (filler sedimentation)

Embodiment 4

?X-6

Barium titanate

2.1

Barium titanate

0.059

35.6

Y-1

79/21

Unstable (filler sedimentation)

Table 8

Paste composition

Dispersion liquid

Inorganic filler

Resin solution

The ratio of inorganic filler/resin

Dispersion stabilization

Form

Average grain diameter (μ m)

Form

Average grain diameter (μ m)

Maximum/minimum (ratio)

Epoxy resin

Volume ratio

Embodiment 43

X-2

Barium titanate

0.5

Barium titanate

0.060

8.3

Y-1

79/21

Stable

Embodiment 44

X-7

Barium titanate

0.5

Strontium titanates

0.045

11.1

Y-1

79/21

Stable

Embodiment 45

X-8

Barium titanate

0.5

Titanium oxide

0.2

2.5

Y-1

81/19

A little instability (aggegation)

Embodiment 46

X-9

Plumbous class filler

0.9

Barium titanate

0.059

15.3

Y-1

86/14

Stable

Comparative example 4

-

Y-1

0/100

-

Comparative example 5

X-10

Barium titanate

0.5

-

-

-

Y-1

79/21

Stable

Comparative example 6

X-11

Barium titanate

7

Barium titanate

0.5

14

Y-1

79/21

Unstable (filler sedimentation)

Comparative example 7

X-12

Barium titanate

40

Barium titanate

2.1

19

Y-1

79/21

Unstable (filler sedimentation)

Comparative example 8

X-13

Barium titanate

20

Barium titanate

2.1

9.5

Y-1

79/21

Unstable (filler sedimentation)

Comparative example 9

-

Barium titanate

0.059

Strontium titanates

0.045

1.3

Y-1

79/21

Unstable (filler sedimentation)

Table 9

	The high dielectric composition
							Thickness (μ m)	Coefficient of linear expansion (ppm/ ℃)	Jie Diantexing @1MHz			The evaluation score of PCT test back gridiron pattern test
	Dielectric constant	Dielectric loss angle tangent (%)	Static capacity (nF/cm 2)
				Embodiment 31	10	18			55	3.3	4.9		10
Embodiment 32	10	17	98				4.4	8.7				10
				Embodiment 33	10	16			110	4.4	9.7		10
Embodiment 34	10	16	109				4.6	9.7				10
				Embodiment 35	10	16			98	6.2	8.7		8
Embodiment 36	10	16	75				8.3	6.6				4
				Embodiment 37	10	16			106	2.9	9.4		10
Embodiment 38	10	16	114				2.2	10.1				10
				Embodiment 39	10	16			93	2.8	8.2		10
Embodiment 40	10	16	102				2.8	9.0				10
				Embodiment 41	10	16			135	3.7	12.0		10

Embodiment 42

10

16

150

4.1

13.3

10

Table 10

	The high dielectric composition
							Thickness (μ m)	Coefficient of linear expansion (ppm/ ℃)	Jie Diantexing @1MHz			The evaluation score of PCT test back gridiron pattern test
	Dielectric constant	Dielectric loss angle tangent (%)	Static capacity (nF/cm 2)
				Embodiment 43	10	16			115	2.9	10.2		10
Embodiment 44	10	16	91				3.9	8.1				10
				Embodiment 45	10	15			47	2.6	4.2		10
Embodiment 46	10	15	80				3.5	7.1				10
				Comparative example 4	10	53			4	2.8	0.3		10
Comparative example 5	10	25	72				6.8	6.4				8
				Comparative example 6	10	32			The measured value instability can't be measured				6
Comparative example 7	10	36	The measured value instability can't be measured				6
						Comparative example 8		10	35	The measured value instability can't be measured			6
Comparative example 9	Because the filler aggegation does not make paste

Claims (7)

1. dielectric composition, it is the dielectric composition that contains inorganic filler and resin, it is characterized in that, inorganic filler has 2 kinds of average grain diameters at least, average grain diameter maximum in the described average grain diameter is 0.1～5 μ m, with respect to minimum average particle diameters, maximum average grain diameter is its 3 times or more than it, the total volume of the cumulative volume that forms branch admittedly with respect to the cumulative volume and the resin of inorganic filler, the ratio Vf of the cumulative volume of inorganic filler satisfies 70%～95%, and voidage is 30 volume % or below it.

2. dielectric composition as claimed in claim 1, inorganic filler are at least a kind that is selected from titanium dioxide class, barium titanate class, metatitanic acid barium zirconate class, strontium titanates class, calcium titanate class, bismuth titanates class, magnesium titanate class, barium neodymium titanate class, barium titanate tin class, magnesium niobic acid barium class, magnesium barium tantalate class, lead titanates class, lead zirconates class, lead zirconate titanate class, lead niobate class, magnesium lead niobate class, nickel lead niobate class, lead tungstate class, artificial schellite class, the magnesium lead tungstate class.

3. dielectric composition as claimed in claim 1, described resin contains heat-curing resin.

4. dielectric composition as claimed in claim 1, described resin are epoxy resin.

5. dielectric composition as claimed in claim 1 contains the compound with phosphate skeleton.

6. a capacitor uses the described dielectric composition of claim 1.

7. the described dielectric composition of claim 1 is used in a light wiring.