JPH083365A - Molding resin composition - Google Patents

Abstract

(57) [Summary] [PROBLEMS] To provide a molding resin composition which has excellent flowability, low hygroscopicity, and low thermal expansion coefficient. [Structure] Spherical powder (x component) having an average particle size of 0.1 μm or more and less than 1.5 μm in a resin (eg, epoxy resin)
And a spherical powder having an average particle size of 2 μm or more and less than 10 μm (y component), a spherical powder having an average particle size of 20 μm or more and less than 70 μm (z component), or a filler composed of these and crushed powder (m component) The proportion of each x, y, z component in the total volume of x, y, z components is 10% by volume or more and 22% by volume or less, 21% by volume or more and 66% by volume or less, 24% by volume or more 57 Volume% or less, the proportion of the m component in the filler is 1% by weight or more and less than 30% by weight, and the proportion of the filler in the entire composition is 70% by weight or more 9
A resin composition for molding which is 4% by weight or less.

Description

Detailed Description of the Invention

[0001]

FIELD OF THE INVENTION The present invention relates to a filler-containing resin composition suitable for injection molding and transfer molding.
The present invention relates to an epoxy resin composition useful as a sealing material for electronic parts.

[0002]

2. Description of the Related Art Recently, LSIs, ICs, transistors, etc.
Transfer molding of an economically useful epoxy resin composition is performed for sealing a semiconductor. In particular, recently, surface mounting of LSIs has been performed, and the number of cases in which a semiconductor package is directly immersed in a solder bath at the time of mounting on a semiconductor substrate is increasing. At this time, since the sealed package is exposed to a high temperature of 200 ° C. or higher, the moisture absorbed in the sealed package expands to cause cracks,
Due to the stress due to thermal stress, peeling occurs between the element or metal frame and the interface of the sealing material. There is a problem that a defect of an element occurs due to the influence of cracks and moisture invading from a peeling interface. Therefore, the resin sealing material is required to have low moisture absorption and crack resistance. At present, epoxy compounds such as glycidyl ether compound of o-cresol novolac and glycidyl ether compound of tetramethyl biphenol are usually used. An inorganic filler such as silica is added to these compounds to form a sealing material, and as a recent technological trend, studies have been made to increase the content of the filler. For example, by increasing the content of silica-based filler to reduce the amount of moisture absorption derived from the resin, and by making the thermal expansion coefficient of the silicon chip and the semiconductor package close to each other, the stress generated during heating is relaxed. Measures to avoid the occurrence of are becoming effective.

From the above technical trend, a method of increasing the content of the silica filler as much as possible is effective, but there is an upper limit in practice. For example, when a single spherical filler close to an ideal single dispersion state is used, in the case of an epoxy resin encapsulant, the flow at the time of heating and melting the encapsulant is about 80% by weight when the content of the encapsulant is about 80% by weight. It becomes extremely short. At 84% by weight, the fluidity is virtually lost and it becomes impossible to seal the element in the mold. In order to avoid this, a multi-component filler is usually used. However, when the filler is highly filled, there is a problem in that the actual flow is reduced to less than half by just increasing the filling amount by a few%, which may make it impractical.

[0004]

SUMMARY OF THE INVENTION An object of the present invention is to provide a molding resin composition having excellent flowability, low hygroscopicity and low thermal expansion coefficient.

[0005]

As a result of intensive investigations, the present inventors have found that a resin composition containing a filler having a specific composition achieves the object of the present invention, and has completed the present invention. I arrived. That is, the present invention is as follows.

(1) Spherical powder (x component) having an average particle size of 0.1 μm or more and less than 1.5 μm and an average particle size of 2 μm in a resin
A spherical powder having a particle size of m or more and less than 10 μm (y component) and a spherical powder having an average particle size of 20 μm or more and less than 70 μm (z component) are contained, and the filler occupies the total volume of the x, y and z components. The proportions of the x, y, and z components are 10% by volume or more and 22% by volume or less, 21% by volume or more and 66% by volume or less, and 24% by volume or more and 57% by volume or less, respectively, and the proportion of the filler in the entire composition. Is 70% by weight or more and 94% by weight or less, a molding resin composition.

(2) Spherical powder (x component) having an average particle size of 0.1 μm or more and less than 1.5 μm in the resin, and an average particle size of 2 μm
m or more and less than 10 μm spherical powder (y component), and an average particle size of 20 μm or more and less than 70 μm spherical powder (z component),
It contains a filler composed of crushed powder (m component),
The proportion of each x, y, z component in the total volume of the x, y, z components is 10% by volume or more and 22% by volume or less, 21
Volume% or more and 66 volume% or less, 24 volume% or more and 57 volume%
Below, the proportion of the m component in the filler is 1% by weight.
A resin composition for molding, which is not less than 30% by weight and the proportion of the filler in the entire composition is not less than 70% by weight and not more than 94% by weight.

(3) An epoxy resin, a phenolic curing agent, a curing accelerator, and a silica powder filler composed of x, y, z and m components as essential components, and the filler is 83% by weight or more based on the total composition. Containing 93 wt% or less,
175 ℃ × 70kg according to EMMI-1-66 standard
The resin composition for molding according to the above (2), which has a spiral flow of 20 inches or more as measured in / cm ² .

The contents of the present invention will be specifically described below.
Examples of the spherical powder used in the present invention include silica, alumina, aluminum nitride, silicon nitride, silicon carbide, silica sand, silica stone powder, talc, white carbon, aerosil, wollastonite, mica, clay, glass sphere, and metal. Spherical powders such as fused silica powders, crystalline silica powders, and alumina powders are preferable from the viewpoint of the coefficient of thermal expansion and high purity, such as spheres.

The shape of the spherical powder may be a substantially spherical shape having no aspect ratio and an aspect ratio of 1.0 to 1.2.
Those having a sphericity of about the level of commercially available spherical silica powder produced by the thermal spraying method or the sol-gel method are preferable, but those closer to a true sphere are more preferable. Further, when the spheroidizing treatment is difficult, a spherical powder can be obtained by pulverizing it into fine particles and then adding a binder by a mechanochemical method to spheroidize.

The crushed powder may have any shape such as a polyhedron having corners. Among them, amorphous or crystalline crushed quartz powder obtained by crushing synthetic or natural quartz lumps is suitable, and specifically fused crushed silica is suitable.

The spherical powder used in the present invention comprises three groups of x, y and z components. x, y, and z components each have an average particle size of 0.1 μm or more and less than 1.5 μm, and an average particle size of 2 μm or more 1
It is less than 0 μm and the average particle size is 20 μm or more and less than 70 μm. The particle size dispersion of each spherical powder used in the present invention is preferably narrow, and more preferably close to a single dispersion. For this reason, it is preferable to use those in which the particle diameters of all the x, y, and z components have been adjusted by classification. The average particle size in the present invention is defined as the particle size value when the weight accumulation is 50% when the particle size distribution is measured using a particle size distribution measuring device such as a laser scattering particle size distribution meter.

The mixing ratio of the spherical powders x, y, and z components is 10% by volume or more and less than 22% by volume and 21% by volume, respectively, in the ratio of the volume of x, y, and z components to the total volume of x and y and z components. It is above 66% by volume and below 24% by volume and below 57% by volume.

The above volume% in the present invention is calculated by dividing the weight of each of the x, y and z components by the true specific gravity of each component as the volume of each component. In general,
The apparent volume of particles having a particle size distribution varies depending on how the particles are filled in the measurement container and before and after mixing different kinds of particle aggregates. Therefore, in the present invention, the apparent volume is not used for calculating the volume% of each component of the particle assembly.

Crushed powder (m component) used in the present invention
Has an average particle size of 1 μm or more and less than 70 μm, preferably 1 μm
Those having a size of m or more and less than 30 μm are used. The mixing ratio of the crushed powder (m component) is defined such that the ratio of the weight of the m component to the total weight of the spherical powder x, y, z components and the crushed powder m component is 1% by weight or more and less than 30% by weight. If the compounding amount is less than this range, the effect of reducing burrs and flashes (resin thin film due to resin exudation) generated by the type of resin, the shape of the sealing device and the mold is poor, and if it exceeds this range, the resin composition The flowability of goods is reduced.

It is preferable that the filler used in the present invention is thoroughly mixed in advance. Specifically, the mixing can be performed by using a device such as a mixer or a cokneader that uses a rotary blade or air, or a device that vibrates, shakes, or rotates the container.
To determine whether the fillers are well mixed, it is advisable to measure the particle size distributions of the samples at different locations and see if they are substantially the same. Further, if necessary, the filler may be pretreated with a coupling agent or a resin before use. As a treatment method, there are a method of distilling off the solvent after mixing with a solvent, and a method of directly blending with a filler and treating with a mixer.

The amount of the filler of the present invention used is 70% by weight or more and 94% by weight or less, preferably 8% by weight, based on the total composition.
It is 3% by weight or more and 93% by weight or less. If it is less than this range, the effect of reducing the hygroscopicity and thermal expansion coefficient derived from the resin is small, and if it exceeds this range, the flowability is impaired.

The resin used in the present invention is thermoplastic,
Alternatively, a thermosetting resin may be used. In particular, a resin for semiconductor encapsulant, which can take advantage of high filling of the filler, is suitable, and among them, a thermosetting resin, particularly an epoxy resin is suitable.

Specific examples of the epoxy resin include polyphenols and polyphenols which are reaction products of phenols such as phenol, o-cresol and catechol, naphthols such as hydroxynaphthalene and dihydroxynaphthalene, and aldehydes such as formaldehyde. Polyphenols containing trityl skeleton, phenol, o-cresol, and catechol obtained by condensation of naphthol-based novolac resins, phenols such as phenol, o-cresol, and methyl-t-butylphenol with aromatic aldehydes such as hydroxybenzaldehyde. Polyaralkylphenol resins and polyaralkylnaphtho, which are reaction products of phenols such as naphthols such as hydroxynaphthalene and dihydroxynaphthalene, and xylylenedichloride. And resins, phenol, o- cresol, phenol and hydroxy naphthalenes of catechol, naphthols dihydroxy naphthalene,
Alicyclic hydrocarbon-containing polyphenol resins and polynaphthol resins, which are reaction products with unsaturated alicyclic hydrocarbons such as dicyclopentadiene and limonene, phloroglysin, tris- (4-hydroxyphenyl) -methane , 1,
1,2,2, -Tetrakis (4-hydroxyphenyl) ethane, 1,3-bis [bis (4-hydroxyphenyl) methyl] benzene, 1,4-bis [bis (4-hydroxyphenyl) methyl] benzene, etc. A glycidyl ether compound derived from cyclic phenols such as trivalent or higher phenols and calixarene having a basic skeleton,

Bisphenol A, bisphenol F, hydroquinone, resorcin, dihydroxynaphthalene,
Bis (4-hydroxyphenyl) menthane, bis (4-
(Hydroxyphenyl) dicyclopentane, 4,4′-dihydroxybenzophenone, bis (4-hydroxyphenyl) ether, bis (4-hydroxy-3-methylphenyl) ether, bis (3,5-dimethyl-4-hydroxyphenyl) Ether, bis (4-hydroxyphenyl) sulfide, bis (4-hydroxy-3-methylphenyl) sulfide, bis (3,5-dimethyl-4-hydroxyphenyl) sulfide, bis (4-hydroxyphenyl) sulfone, bis ( 4-hydroxy-3-methylphenyl) sulfone, bis (3,5-dimethyl-4-hydroxyphenyl) sulfone, 1,1-bis (4-hydroxyphenyl) cyclohexane, 1,1-bis (4-hydroxy-3) -Methylphenyl) cyclohexane, 1,1-bis (3,5-dimethyl-4-hydroxyphenyl) ) Cyclohexane, 4,4'-dihydroxybiphenyl, 4,4'-dihydroxy-3,3 ', 5,5'-tetramethylbiphenyl, bis (hydroxynaphthyl) methane, 1,1'-binaphthol,
Glycidyl ether compounds derived from dihydric phenols such as 1,1'-bis (3-t-butyl-6-methyl-4-hydroxyphenyl) butane or halogenated bisphenols such as tetrabromobisphenol A Diglycidyl ether compound, a polyhydric phenol glycidyl ether compound obtained by a condensation reaction of a phenol and an aromatic carbonyl compound,

P-aminophenol, m-aminophenol, 4-aminometacresol, 6-aminometacresol, 4,4'-diaminodiphenylmethane, 3,3'-diaminodiphenylmethane, 4,4'-diaminodiphenylether, 3 , 4'-Diaminodiphenyl ether, 1,4-bis (4-aminophenoxy) benzene, 1,4-bis (3-
Aminophenoxy) benzene, 1,3-bis (4-aminophenoxy) benzene, 1,3-bis (3-aminophenoxy) benzene, 2,2-bis (4-aminophenoxyphenyl) propane, p-phenylenediamine, m-phenylenediamine, 2,4-toluenediamine, 2,6-toluenediamine, p-xylylenediamine, m-xylylenediamine, 1,4-cyclohexanebis (methylamine), 1,3-cyclohexanebis (methyl Amine-based epoxy resin derived from amine, etc.,

Glycidyl ester compounds derived from aromatic carboxylic acids such as p-oxybenzoic acid, m-oxybenzoic acid, terephthalic acid and isophthalic acid, hydantoin epoxy compounds derived from 5,5-dimethylhydantoin, etc. , 2,2-bis (3,4-epoxycyclohexyl) propane, 2,2-bis [4- (2,3-epoxypropyl) cyclohexyl] propane, vinylcyclohexenedioxide, 3,4-epoxycyclohexylmethyl-3 There are alicyclic epoxy resins such as 1,4-epoxycyclohexanecarboxylate, aliphatic epoxy resins obtained by oxidizing double bonds in unsaturated hydrocarbon compounds such as polybutadiene, and N, N-diglycidylaniline. One or more of these epoxy resins are used. Among them, polyphenol-based novolac resins, trityl skeleton-containing polyphenols, polyaralkylphenol-based resins, alicyclic hydrocarbon-containing polyphenol resins, polyphenols and polyvalent phenols obtained by condensation reaction of phenols and aromatic carbonyl compounds Glycidyl ether compounds such as naphthol are preferable in terms of Tg, adhesiveness and strength, and dihydroxynaphthalene, bis (4-hydroxyphenyl) ether, bis (3,5-dimethyl-4)
-Hydroxyphenyl) sulfide, 1,1-bis (4-
(Hydroxy-3-methylphenyl) cyclohexane, 4,
4'-dihydroxybiphenyl, 4,4'-dihydroxy-3,
Diglycidyl ether compounds of 3 ', 5,5'-tetramethylbiphenyl, bis (4-hydroxyphenyl) menthane, and bis (4-hydroxyphenyl) dicyclopentane are preferable from the viewpoint of viscosity, adhesiveness and low hygroscopicity.

Examples of the resin other than the epoxy resin used in the present invention are as follows.
As a thermosetting resin, an acrylic acid group, a methacrylic acid group,
Vinylbenzyl group, resins having unsaturated bonds such as maleimide groups, cyanates, resins having isocyanate groups, combinations of benzocyclobutene and unsaturated bonds, etc.
Resins using the Diels-Alder reaction, in the presence of platinum catalyst,
Examples thereof include resins that utilize the reaction between siloxanes containing hydrogen silicide and unsaturated bonds.

Examples of the thermoplastic resin include heat-resistant resins such as wholly aromatic polyester, polyamideimide, polyimide, polyetherimide, polyethersulfone and polyetheretherketone.

Known epoxy curing agents can be used in the present invention. Examples of these are phenols such as phenol, o-cresol and catechol, hydroxynaphthalenes, polyphenols and polynaphthol novolac resins which are reaction products of naphthols such as dihydroxynaphthalene and aldehydes such as formaldehyde, and phenols. , O-cresol, methyl-t-butylphenol, and other phenols, and triphenol skeleton-containing polyphenols obtained by condensation of hydroxybenzaldehyde and other aromatic aldehydes, phenol, o-cresol, catechol, and other phenols, and hydroxynaphthalene , Aralkylphenol resins and polyaralkylnaphthol resins, which are reaction products of naphthols such as dihydroxynaphthalene and xylylene dichlorides, phenol, o-crezo Alicyclic hydrocarbon-containing polyphenol resins which are the reaction products of phenols such as phenol and catechol, naphthols such as hydroxynaphthalene and dihydroxynaphthalene, and unsaturated alicyclic hydrocarbons such as dicyclopentadiene and limonene And polynaphthol resins,

Phloroglysin, tris- (4-hydroxyphenyl) -methane, 1,1,2,2, -tetrakis (4-hydroxyphenyl) ethane, 1,3-bis [bis (4-hydroxyphenyl) methyl] Tribasic or higher phenols having benzene, 1,4-bis [bis (4-hydroxyphenyl) methyl] benzene or the like as a basic skeleton, cyclic phenols such as calixarene, bisphenol A, bisphenol F, hydroquinone, resorcin, dihydroxynaphthalene , Bis (4-hydroxyphenyl) ethane, bis (4-hydroxyphenyl) propane, bis (4-hydroxyphenyl) butane, bis (4-hydroxyphenyl) pentane, bis (4-hydroxyphenyl) hexane, 1,3, 3-trimethyl-1-m-hydroxyphenylindan-5 or 7-ol, Scan (4 - hydroxyphenyl) menthane, bis (4 - hydroxyphenyl)
Dicyclopentane, 4,4'-dihydroxybenzophenone, bis (4-hydroxyphenyl) ether, bis (4-hydroxy-3-methylphenyl) ether, bis (3,5-dimethyl-4-hydroxyphenyl) ether, bis (4-hydroxyphenyl) sulfide, bis (4-hydroxy-3-methylphenyl) sulfide,
Bis (3,5-dimethyl-4-hydroxyphenyl) sulfide, bis (4-hydroxyphenyl) sulfone, bis (4-hydroxy-3-methylphenyl) sulfone,
Bis (3,5-dimethyl-4-hydroxyphenyl) sulfone, 1,1-bis (4-hydroxyphenyl) cyclohexane, 1,1-bis (4-hydroxy-3-methylphenyl) cyclohexane, 1,1-bis (3,5-dimethyl-
4-hydroxyphenyl) cyclohexane, 4,4'-dihydroxybiphenyl, 4,4'-dihydroxy-3,3 ', 5,5'
-Tetramethylbiphenyl, bis (hydroxynaphthyl) methane, 1,1'-binaphthol, 1,1'-bis (3-t
-Butyl-6-methyl-4-hydroxyphenyl) butane and other dihydric phenols or tetrabromobisphenol A and other halogenated bisphenols,

Polycarboxylic acids obtained by condensation reaction of phenols and aromatic carbonyl compounds, polycarboxylic acids such as maleic acid, phthalic acid, nadic acid, methyl-tetrahydrophthalic acid and methyl nadic acid and anhydrides thereof, diaminodiphenylmethane. , Polyamino compounds such as diaminodiphenyl sulfone, diaminodiphenyl ether, phenylenediamine, diaminodicyclohexylmethane, xylylenediamine, toluenediamine, diaminodicyclocyclohexane, dichlorodiaminodiphenylmethane (including isomers), ethylenediamine, hexamethylenediamine, and the like. Examples thereof include active hydrogen-containing compounds capable of reacting with an epoxy group, such as dicyandiamide and tetramethylguanidine. Among them, phenolic novolac resins, naphthol novolac resins,
Phenolic aralkyl resins, naphthol aralkyl resins, alicyclic hydrocarbon-containing polyphenol resins and alicyclic hydrocarbon-containing polynaphthol resins are preferably used from the viewpoint of curability and moisture resistance.

In the epoxy resin composition of the present invention, the mixing ratio of the epoxy curing agent to the epoxy resin is 0.
7 to 1.2 equivalents are preferable, and equivalent addition is more preferable.
If these formulations are extremely deviated from the equivalent formulation, moisture resistance,
It is not preferable because the curability and the like are lowered.

The heat curing method of the epoxy resin composition of the present invention will be described. It becomes possible to easily cure the epoxy resin composition in a short time by using a curing accelerator. It is indispensable especially when it is used as a sealing material. Examples of such catalysts include organic phosphine compounds such as triphenylphosphine, tri-4-methylphenylphosphine, tri-4-methoxyphenylphosphine, tributylphosphine, trioctylphosphine and tri-2-cyanoethylphosphine, tetraphenylphosphonium. Organic phosphonium salts such as tetraphenylborate, tributylamine, triethylamine, tertiary amines such as 1,8-diazabicyclo (5,4,0) undecene-7 and triamylamine, benzyltrimethylammonium chloride, benzyltrimethylammonium hydroxide, Quaternary ammonium salts such as triethylammonium tetraphenylborate, imidazoles, boron trifluoride complex, transition metal acetylacetonate, benzoyl peroxide, di-t
Butyl peroxide, dicumyl peroxide, lauroyl peroxide, acetyl peroxide, methyl ethyl ketone peroxide, cyclohexanone peroxide,
Examples thereof include radical initiators such as t-butyl hydroperoxide and azobisisobutyronitrile, but the invention is not limited thereto. Among these, organic phosphine compounds, imidazoles and salts thereof (specifically, tetraphenylphosphonium tetraphenylborate, 4-methylimidazole tetraphenylborate, etc.) or triethylammonium tetraphenylborate are particularly preferable.

The amount of the curing accelerator used is 100% epoxy resin.
0.1 to 10 parts by weight is used with respect to parts by weight, and more preferably 0.5 to 3 parts by weight. If the amount used is less than this range, molding in a short time becomes difficult and the productivity of the molded product per unit time decreases. On the other hand, if it exceeds this range, the curability at high temperature becomes unnecessarily large, and the operability becomes difficult, and the storage stability of the compound deteriorates.

It is also possible to use a known polymerization inhibitor together in order to adjust the curing speed. For example,
2,6-di-t-butyl-4-methylphenol, 2,2'-
Methylenebis (4-ethyl-6-t-butylphenol), 4,4'-methylenebis (2,6-di-t-butylphenol), 4,4'-thiobis (3-methyl-6-t-butylphenol), hydroquinone Phenols such as monomethyl ether, hydroquinone, catechol, pt
-Polyphenols such as -butylcatechol, 2,5-di-t-butylhydroquinone, methylhydroquinone, t-butylhydroquinone and pyrogallol, phenothiazine compounds such as phenothiazine, benzophenothiazine and acetamidophenothiazine, N-nitrosodiphenylamine, N- There are N-nitrosamine-based compounds such as nitrosodimethylamine.

In the resin composition of the present invention, if necessary, a natural wax, a synthetic wax, a higher fatty acid and a metal salt thereof, a release agent such as paraffin or a colorant such as carbon black, and a silane coupling agent. You may add surface treatment agents, such as an agent. Further, a flame retardant such as antimony trioxide, a phosphorus compound or a brominated epoxy resin may be added for flame retardation. A brominated epoxy resin is particularly preferable for producing a flame retardant effect.

For reducing the stress, for example, various elastomers may be added or reacted in advance and used. Specific examples thereof include addition type or reaction type elastomers such as polybutadiene, butadiene-acrylonitrile copolymer, silicone rubber and silicone oil.

The resin composition thus obtained can be compounded by melt mixing with a general kneader such as a roll or a cokneader.

In order to seal electronic parts such as semiconductors using the resin composition according to the present invention, curing molding may be carried out by a conventionally known molding method such as transfer molding, compression molding or injection molding.

Spiral flow is mentioned as one index showing the flowability of the molding resin composition. The spiral flow of 20 inches or more means that the tip of the cured product of the molding resin composition is 20 inches or more when measured under the conditions of 175 ° C. × 70 kg / cm ² according to the standard of EMMI-1-66. Means reaching the point (EMMI is E
poxy Molding Materials In
Abbreviation for status. American Plastics Industry Association standard. ). If this value is smaller than 20 inches, the transfer molding method, which is generally used, does not require filling of the composition into the mold or excessive use of the amount of compound used at one time, and molding must be performed at high pressure. Will not be obtained. If this value is small, the number of products that can be molded per shot in the mold will be small. This leads to a decrease in productivity per unit time, which is industrially disadvantageous. If the value of the spiral flow is large, not only the number of products per shot will increase, but also the viscosity will increase, so that it is possible to use resin components and modifiers that could not be used normally for higher performance. It means that the range of prescription application is expanded. Thus, ensuring a sufficient spiral flow in the molding resin composition means that a great advantage can be obtained in practical use.

[0037]

EXAMPLES Examples of the present invention will be shown below, but the present invention is not limited thereto. Reference Examples 1 to 10 Spherical silica and crushed fused silica having physical properties such as average particle diameter shown in Table 1 were used, and after compounding in a volume% shown in Table 2,
The mixture was thoroughly mixed to obtain the fillers of Reference Examples 1-10. The average particle size in Table 1 is measured by a laser scattering particle size distribution meter (M
manufactured by Alvern, Master Sizer MS-
Use 20. ) Was used to measure the particle size distribution, and the particle size value of 50% weight accumulation was taken as the average particle size.

[0038]

[Table 1]

[0039]

[Table 2]

Examples 1-5, Comparative Examples 1-5 As the epoxy resin, glycidyl ether compound of 4,4'-hydroxy-3,3 ', 5,5'-tetramethylbiphenyl (melt viscosity 0.1 poise / 150 ℃, manufactured by Sumitomo Chemical Co., Ltd., as a curing agent phenol novolac (trade name Tamanol 759)
, Arakawa Chemical Co., Ltd.), triphenylphosphine as a curing accelerator, carnauba wax as a release agent, a coupling agent (trade name SH-6040, manufactured by Toray Dow Corning Silicone Co., Ltd.) and the fillers of Reference Examples 1 to 20, respectively. Blended in the amounts (g) shown in Tables 3 and 4, kneaded by heating with a roll,
Press molding was performed. Further, post-curing was performed in an oven at 180 ° C for 5 hours to obtain a cured molded product. The glass transition temperature, water absorption, bending strength and moldability of this cured molded product were measured. Regarding the moldability, the appearance of the product such as burrs and surface roughness of the molded product was displayed in three stages of ○, △, and ×. O indicates that there is no problem in practical use, Δ indicates that it is usable but inferior to O, and × indicates that it is not practical.
The results are shown in Tables 3 and 4.

The evaluation method of the cured molded article is as follows. -Spiral flow: According to the standard of EMMI-1-66, it was performed under the condition of 175 ° C x 70 kg / cm ² (unit: inch). Glass transition temperature (Tg), coefficient of thermal expansion: Measured using a thermomechanical analyzer (SHIMADZUDT-30).

Bending strength: Instron universal material testing machine (SHIMADZU) according to JIS K-6911
IS-10T). Water absorption rate: Using a constant temperature and humidity chamber (TABAI PR-2), the weight change of the package in which the simulated element was sealed was measured under the condition of 85 ° C./85% RH.・ Cracking property test: Using eight packages mounted with simulated elements, water was absorbed under conditions of 85 ° C./85% RH × 72 hours, and immediately immersed in a solder bath at 240 ° C. for 30 seconds,
The presence or absence of package cracks was examined.

[0043]

[Table 3]

[0044]

[Table 4]

[0045]

EFFECT OF THE INVENTION The molding resin composition of the present invention exhibits excellent flowability and is highly filled with the filler, so that it has high hygroscopicity and high coefficient of thermal expansion due to the resin of the cured product. Has been reduced. The molding resin composition of the present invention is particularly suitable for a semiconductor encapsulant, but can also be widely applied to other uses that require high filling of the filler.

 ─────────────────────────────────────────────────── ─── Continuation of the front page (72) Inventor Noriaki Saito 6 Kitahara, Tsukuba, Ibaraki Sumitomo Chemical Co., Ltd.

Claims (5)

[Claims] 1. An average particle size of 0.1 μm or more and 1.5 in a resin.
Spherical powder having a particle size of less than μm (x component), spherical powder having an average particle size of 2 μm or more and less than 10 μm (y component), and having an average particle size of 20
It contains a filler made of spherical powder (z component) having a size of at least μm and less than 70 μm, and the proportion of each x, y, z component in the total volume of x, y, z components is 10% by volume to 22 volumes, respectively. % Or less, 21% by volume or more and 66% by volume or less, 24
A molding resin composition, wherein the content of the filler is from 70% by volume to 57% by volume, and the proportion of the filler in the entire composition is from 70% by weight to 94% by weight. 2. An average particle diameter of 0.1 μm or more and 1.5 in the resin.
Spherical powder having a particle size of less than μm (x component), spherical powder having an average particle size of 2 μm or more and less than 10 μm (y component), and having an average particle size of 20
a spherical powder (z component) having a size of at least μm and less than 70 μm, and a filler composed of crushed powder (m component), x,
The proportion of each x, y, z component in the total volume of the y, z components is 10% by volume or more and 22% by volume or less, 21% by volume or more and 66% by volume or less, 24% by volume or more and 57% by volume or less, A molding resin composition in which the proportion of the m component in the total filler is 1% by weight or more and 30% by weight or less, and the proportion of the filler in the entire composition is 70% by weight or more and 94% by weight or less. 3. The spherical powder x, y, z components are made of spherical silica, and the crushed powder m component has an average particle size of 1 μm or more and 30 μm.
The resin composition for molding according to claim 2, which is silica of m or less. 4. The resin according to claim 1, wherein the resin is an epoxy resin.
Alternatively, the molding resin composition according to the item 3. 5. An epoxy resin, a phenolic curing agent, a curing accelerator, and a silica powder filler composed of x, y, z and m components as essential components, and the filler is 83 parts by weight or more and 93 parts by weight or more based on the total composition. Contains less than or equal to parts by weight, EMMI
175 ℃ × 70kg / cm ² according to the standard of -1-66
The molding resin composition according to claim 2 or 3, wherein the spiral flow measured by the method is 20 inches or more.