JPH0841173A - Liquid epoxy resin composition, its production and method of curing same - Google Patents

Abstract

PURPOSE:To obtain a liquid epoxy resin composition having low viscosity and being excellent in handleability, humidity resistance, etc., by mixing an epoxy resin with a curing agent containing a specified compound and an acid anhydride and fused silica. CONSTITUTION:This composition is produced by mixing an epoxy resin (A) (e.g. bisphenol A epoxy resin) with a curing agent (B) containing a naphthalene- skeleton-containing compound (B) represented by the formula and an acid anhydride and fused silica (C). It is desirable that the amount of component C is 10-80wt.% based on the total weight of the composition, that the particle diameter of component C is 20mum or above and that the content of particles having a diameter of 20mum or above and a specific gravity of 0.7-1.5 is at least 50vol.% based on the total amount of particles having diameters of 20mum or above. This composition can be desirably used to form a sealed resin layer by spot sealing and can give a cured product having reduced warpage and high reliability.

Description

Detailed Description of the Invention

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a liquid epoxy resin composition, for example, an adhesive for electronics, particularly a liquid epoxy resin composition for sealing a semiconductor chip directly mounted on a substrate, a method for producing the same, and a method for producing the same. It relates to the curing method.

[0002]

2. Description of the Related Art Epoxy resin compositions have excellent electrical performance and adhesive strength, and are therefore used in various applications in the electric and electronic fields. It is known that the epoxy resin composition uses various curing agents at the time of curing, and that the performance of the cured product greatly varies depending on the type of the curing agent, and the curing agent is properly used depending on the application. For example, in the use of adhesives and laminates, amine-based curing agents are used because adhesion is the most important, and in casting applications, acid anhydrides are used from the viewpoint of electrical performance and low viscosity. Phenolic curing agents are used for sealing materials from the viewpoint of water resistance.

Conventionally, amines and acid anhydrides have been known as curing agents for liquid epoxy resin compositions such as solventless adhesives, sealing materials for electric and electronic parts, paints and the like. When a phenol-based curing agent is used, a phenol novolac resin is generally used, and the liquid epoxy resin composition has a large molecular weight and the addition amount of the phenol novolac resin curing agent to the epoxy resin is 50 PHR or more, which is large. The viscosity of is so high that it cannot be put to practical use. However, in terms of the balance of physical properties such as adhesiveness, water resistance, and electrical performance, the phenolic curing agent is the most excellent curing agent. That is, since it is difficult to liquefy, phenolic curing agents can generally be used only for solid molding materials. Amine-based and acid anhydride-based curing agents are easy to liquefy, but have the following problems. That is, when an amine-based curing agent is used, the hygroscopicity is high because a tertiary amine structure exists in the crosslinked structure of the cured product. When an acid anhydride-based curing agent is used, long-term water resistance is poor because the ester structure in the crosslinked structure of the cured product is easily chemically hydrolyzed, and the acid anhydride group of the curing agent and the epoxy resin The cured product is inferior in adhesiveness because the alcoholic hydroxyl group that contributes to adhesion is less likely to be by-produced by the reaction with the epoxy group.

Since recent electronic parts tend to be higher in density and thinner, a bare chip is mounted from a conventional transfer molded package and sealed with a liquid sealing material.
So-called chip-on-board (COB) and TAB (Tap)
e Automated Bonding) is being replaced. As a conventional liquid encapsulating material, an epoxy resin composition using an amine-based or acid anhydride-based curing agent is predominant because of its limited viscosity. However, the liquid encapsulant composed of the epoxy resin composition using the amine-based or acid anhydride-based curing agent is more than the transfer molding material composed of the epoxy resin composition using the phenol novolac resin curing agent described above. Poor overall reliability. Therefore, it is strongly desired to improve the reliability of the liquid sealing material. Therefore, in order to compensate for the drawback of high viscosity of the epoxy resin composition using a phenolic curing agent, the use of a solvent,
Although the handling of the liquid encapsulating material has been facilitated by using it together with an amine-based curing agent or an acid anhydride-based curing agent, the liquid sealing material has not yet reached a satisfactory stage. Therefore,
The inventors of the present application proposed a liquid epoxy resin composition containing allyl etherified naphthalene as a curing agent in Japanese Patent Application No. 4-284864. Recently, HIC and PLCC
In addition to the need for encapsulating a large area for the above-mentioned application, the opportunity for encapsulating a large area is increasing with the increase in size of the chip for ordinary applications. However, when a large area is sealed, the filler on the upper and lower surfaces of the encapsulant is different from the difference in expansion and contraction between the substrate and the cured product of the liquid epoxy resin composition, or the difference in the sedimentation speed of the filler. Due to the difference in the content and the like, warpage occurs in this cured product, which not only causes a problem at the time of mounting, but also easily causes microscopic interface peeling between the cured product and the chip due to the warp stress, which causes a decrease in moisture resistance. There was a problem. In order to prevent the settling of the filler, it is better to reduce the specific gravity and particle size of the filler, but many fillers with a low specific gravity have a poor balance with other characteristics. If it is unnecessarily reduced, the specific surface area will be large, and it will not be possible to add a large amount of filler, the linear expansion coefficient of the cured product will be large, the difference between expansion and contraction with the substrate will widen, and it will rather warp. There is a problem,
We are increasing the amount of filler and lowering the elasticity,
It has not achieved sufficient results.

[0005]

SUMMARY OF THE INVENTION The present invention has been made in view of the above facts, and an object thereof is to form a resin sealing layer by spot sealing with low viscosity and good handleability. The present invention provides a liquid epoxy resin composition which is suitable for use as a liquid epoxy resin composition, has a small warpage, and is excellent in moisture resistance, heat resistance, and the like, and is highly reliable.

[0006]

The liquid epoxy resin composition according to claim 1 of the present invention is a liquid epoxy resin composition which is liquid at room temperature and contains the epoxy resin, a curing agent and an inorganic filler. And a compound having a naphthalene skeleton represented by the following general formula and an acid anhydride, wherein the inorganic filler contains fused silica.

[0007]

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A liquid epoxy resin composition according to a second aspect of the present invention is a liquid epoxy resin composition which is liquid at room temperature and contains an epoxy resin, a curing agent and an inorganic filler, and has the above general formula as the curing agent. It is characterized in that it contains a compound having a naphthalene skeleton represented and an aromatic amine, and the above-mentioned inorganic filler contains fused silica.

A liquid epoxy resin composition according to a third aspect of the present invention is characterized in that the content of the inorganic filler is 10 to 80% by weight based on the total amount of the liquid epoxy resin composition. .

In a liquid epoxy resin composition according to a fourth aspect of the present invention, the inorganic filler has particles having a particle size of 20 μm or more, a particle size of 20 μm or more, and a specific gravity of 0.7 to.
The content of the particles of 1.5 is 50% by volume or more with respect to the total amount of the particles having a particle diameter of 20 μm or more.

A liquid epoxy resin composition according to a fifth aspect of the present invention has a particle size of 20 μm or more and a specific gravity of 0.7.
The inorganic filler of particles of ˜1.5 is characterized by being hollow silica balloons.

A liquid epoxy resin composition according to a sixth aspect of the present invention has a particle size of 20 μm or more and a specific gravity of 0.7.
The inorganic filler particles of ˜1.5 are methyl silicates.

A method for producing a liquid epoxy resin composition according to a seventh aspect of the present invention is to provide a kneaded product obtained by kneading a compounded product of a liquid epoxy resin composition containing an epoxy resin, a curing agent and fused silica with the above hollow silica. A feature is that a balloon is added later and mixed.

A method for curing a liquid epoxy resin composition according to an eighth aspect of the present invention is a method in which the liquid epoxy resin composition according to the first to sixth aspects is preheated at 80 to 130 ° C. and then 150 to 200. It is characterized by heat treatment at ℃.

The present invention will be described in detail below. The matrix resin constituting the liquid epoxy resin composition of the present invention is an epoxy resin having two or more epoxy groups in one molecule, for example, bisphenol A type epoxy resin, bisphenol F type epoxy resin, novolac type. Epoxy resin, halogenated epoxy resin, glycidyl ester type epoxy resin, alicyclic epoxy resin, naphthalene type epoxy resin, biphenyl type epoxy resin and the like are used. These epoxy resins can be selected within the range where the epoxy resin composition is liquefied, and are not limited to the above epoxy resins.

As a curing agent, it is essential to use a compound having a naphthalene skeleton represented by the above general formula (hereinafter referred to as compound A). This compound A is synthesized from a compound (1,6 dioxynaphthalene) represented by the following general formula, which is an aromatic compound containing two non-allylated phenolic hydroxyl groups (hereinafter referred to as compound a). Is possible.

[0017]

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The non-allylated compound a is a solid having a high melting point, and like the phenol novolac resin, it cannot give good flowability to the epoxy resin composition even when used as a curing agent. However, allylation of compound a results in allylated compound A having a significantly reduced melting point. By using this compound A as a curing agent, a liquid epoxy resin composition having a low viscosity at room temperature can be obtained. However, when the curing agent is only the compound A, the liquid epoxy resin composition cannot be cured unless it is treated at a temperature of about 150 to 160 ° C. for several hours, so that the filler is apt to settle and warp is likely to occur. .
Therefore, the compound A is used in combination with the acid anhydride or the aromatic amine as the curing agent. That is, by using the compound A as a curing agent, a low-viscosity liquid epoxy resin composition at room temperature can be obtained, and by using an acid anhydride or an aromatic amine in combination, the average molecular weight of the epoxy resin can be reduced in a short time. And the solution viscosity of the liquid epoxy resin composition is increased, the sedimentation of the filler can be suppressed and the warpage can be improved. The ratio of the contents of the compound A and the acid anhydride or the aromatic amine is 1: 2 to 4: 1 in equivalent conversion.
Is preferred. That is, when the content ratio of the compound A and the acid anhydride or the aromatic amine is more than 1: 2, the hydrolyzability becomes remarkable or the water absorption rate is high. When the content of the compound A is higher than 4: 1, the sufficient effect for improving the warp cannot be obtained.

Examples of the acid anhydride include phthalic anhydride, tetrahydrophthalic anhydride, methyltetrahydrophthalic anhydride, hexahydrophthalic anhydride, methylhexahydrophthalic anhydride, succinic anhydride and endomethylenetetrahydrophthalic anhydride. However, it is not limited thereto.

Examples of aromatic amines include, but are not limited to, diaminodiphenylmethane, diaminodiphenylsulfone, diaminodiphenyl ether, and formalin condensates of aniline.

The content of the inorganic filler is preferably 10 to 80% by weight, more preferably 30 to 75% by weight, based on the total amount of the liquid epoxy resin composition in order to suppress expansion and contraction with the substrate. %. That is, the content of the inorganic filler is 8 with respect to the total amount of the liquid epoxy resin composition.
When it exceeds 0% by weight, the viscosity of the liquid epoxy resin composition becomes too high, and when it is less than 10% by weight, the effect of lowering the linear expansion cannot be obtained. As this inorganic filler,
If necessary, the surface of the inorganic filler containing fused silica can be surface-treated with a coupling agent. Among the inorganic fillers, the fused silica referred to in the present invention has a specific gravity of about 2.2, which is small, so that a good cured product with less warpage than crystalline silica, alumina, calcium carbonate, etc., which has a large specific gravity, can be obtained. And has an excellent balance with other physical properties.

When the inorganic filler contains particles having a particle size of 20 μm or more, the content of particles having a particle size of 20 μm or more and a specific gravity of 0.7 to 1.5 is 20 μm or more. It is preferably 50% by volume or more with respect to the total amount of particles, the particle size is 20 μm or more, and the specific gravity is 1.0 to
It is more preferable that the content of the particles of 1.4 is 50% by volume or more with respect to the total amount of the particles having the particle diameter of 20 μm or more. That is, particles having a particle size of 20 μm or less cause little warpage because they settle slowly, and the content of particles having a particle size of 20 μm or more and a specific gravity of 0.7 to 1.5 is as described above. For the total amount of particles with a particle size of 20 μm or more,
If it is less than 50% by volume, the effect of reducing the warp is small.
In the present invention, the particles having a specific gravity of 0.7 to 1.5 do not include the fused silica.

When the particle size is 20 μm or more and the specific gravity is 0.
It is preferred that the inorganic filler of 7-1.5 particles is a hollow silica balloon or methyl silicate. When a hollow silica balloon is used, since it may be destroyed during kneading, as a method for producing a liquid epoxy resin composition, the hollow silica balloon is not put in the compounded product before kneading, and the epoxy resin is cured. It is preferable that the hollow silica balloon is post-added to and mixed with a kneaded product obtained by kneading a compounded product of a liquid epoxy resin composition containing an agent and fused silica. That is, by post-adding and mixing this hollow silica balloon, the destruction of the hollow silica balloon is almost eliminated, and the effect of reducing warpage is increased.

The liquid epoxy resin composition of the present invention may be used in an amount of 80-
After heat treatment at 130 ℃ for 10 minutes or more, 150 to 200 ℃
It is preferable to heat-treat. That is, in the liquid epoxy resin composition of the present invention, by setting the temperature to 80 to 130 ° C., it is possible to polymerize or cure the liquid epoxy resin composition by the reaction between the epoxy resin and the acid anhydride or the aromatic amine. is there. Liquid epoxy resin composition 80-130
By pre-treating in the low temperature range of ℃, the viscosity of the liquid epoxy resin composition is relatively large, the sedimentation of the filler is suppressed, and the heating of 150 to 200 ℃ which causes the reaction of the next step by the transfer of the compound A. Since the viscosity of the liquid epoxy resin composition at the stage can be significantly increased, the sedimentation of the filler can be further suppressed, so that the cured product of the liquid epoxy resin composition is less likely to warp.

As the curing accelerator, a phosphorus-based or tertiary amine-based curing accelerator is used, and the curing accelerator is not particularly limited. Furthermore, if necessary, a reaction diluent, a flame retardant, a pigment, a dye, a flexibility-imparting agent, a release agent, etc. can be added.

[0026]

Regarding the cause of warpage, not only the cause of expansion and contraction of the substrate and the cured product of the liquid epoxy resin composition, but also the inclusion of the inorganic filler on the upper and lower surfaces of the cured product due to the sedimentation of the inorganic filler. It is caused by the difference in quantity. That is,
In a liquid epoxy resin composition that needs to be liquid at room temperature, when the temperature is elevated for curing, the liquid epoxy resin composition has a very low viscosity before the polymerization occurs by the reaction, and therefore the inorganic material having a large specific gravity is used. The filler settles, resulting in warpage.

Settling velocity v of spherical particles floating in a liquid
Is derived from the Navier-Stokes equation and is expressed by the following equation.

[0028] Here, ρ; particle specific gravity, ρ ₀ ; solution specific gravity, g; gravitational acceleration D; particle size, η; solution viscosity In order to prevent the sedimentation of the inorganic filler, (ρ−ρ ₀ ) is set small, that is, the solution. It is preferable that the difference between the specific gravity ρ ₀ and the particle specific gravity ρ is small and the particle diameter D of the inorganic filler is small. However, fillers with a small specific gravity often have a poor balance with other properties, and if the particles are made too small, the specific surface area increases, and a large amount of inorganic filler cannot be added, resulting in a linear expansion coefficient of the cured product. Becomes larger, the difference in expansion and contraction between the cured product and the substrate increases, and the warpage becomes larger.

In the liquid epoxy resin composition according to any one of claims 1 to 3, by using the compound A as a curing agent, a liquid epoxy resin composition having a low viscosity at room temperature can be obtained. By using together with the group amine, the average molecular weight of the epoxy resin is raised in a short time and the solution viscosity of the liquid epoxy resin composition is raised, whereby the sedimentation of the filler is suppressed. Moreover, by using fused silica having a relatively low specific gravity of about 2.2 as the inorganic filler, the sedimentation speed of the inorganic filler is slowed down, and the sedimentation of the inorganic filler results in the upper and lower surfaces of the cured product. The difference in content of the inorganic filler can be reduced.

In the liquid epoxy resin composition according to any one of claims 4 to 6, by using an inorganic filler having a smaller specific gravity, sedimentation of the filler can be suppressed. That is, the specific gravity of the inorganic filler having a large particle size is reduced to a particle size of 20 μm or more contained in the inorganic filler, and the specific gravity is 0.7 to 1.
By setting the content of the particles such as the hollow silica balloon of 5 or methyl silicate to 50% by volume or more based on the total amount of the particles having a particle size of 20 μm or more, the sedimentation rate of the inorganic filler can be slowed and the inorganic filling can be performed. It is possible to further reduce the difference in the content of the inorganic filler on the upper and lower surfaces of the cured product due to the sedimentation of the agent.

In the method for producing a liquid epoxy resin composition according to claim 7, the hollow silica balloon is added to a kneaded product obtained by kneading a compounded product of the liquid epoxy resin composition containing an epoxy resin, a curing agent and fused silica. Since it is added and mixed, the hollow silica balloon is not broken and the state of low specific gravity is maintained.

In the method for curing a liquid epoxy resin composition according to claim 8, the liquid epoxy resin composition is 80 to 130
By pre-treating in the low temperature range of ℃, the viscosity of the liquid epoxy resin composition is relatively large, the sedimentation of the filler is suppressed, and the heating of 150 to 200 ℃ which causes the reaction of the next step by the transfer of the compound A. Since the viscosity of the liquid epoxy resin composition at the stage can be significantly increased, the sedimentation of the filler can be further suppressed.

[0033]

EXAMPLES The present invention will be specifically described below with reference to Examples and comparison with Comparative Examples.

Examples 1 to 15 As the epoxy resin, a bisphenol A type epoxy resin (YD812) is used.
5: Toto Kasei Co., Ltd.) and a phenol novolac type epoxy resin (YDPN180P: Toto Kasei Co., Ltd.) were used.

The above compound A was used as a curing agent, B-650 manufactured by Dainippon Ink and Co., Inc. as an acid anhydride, and diaminodiphenylmethane or diaminodiphenylsulfone as an aromatic amine. As the compound A, the compound A obtained in the synthesis example disclosed in Japanese Patent Application No. 4-284764 by the present inventors was used. That is, the compound A is synthesized by using the compound a which is the compound (1,6 dioxynaphthalene) represented by the above general formula. 80 g of compound a 3
After dissolving in 200 ml of dehydrated acetone in a one-necked flask, 140 g of potassium carbonate was added to obtain a phenolate, and 140 g of allyl bromide was added dropwise at room temperature (about 10 to 30 ° C.) in 20 minutes, and acetone was added for 5 hours. Was refluxed and reacted. After completion of the reaction, the mixture was transferred to a 1 liter beaker, 500 ml of deionized water was added, and the mixture was extracted twice with 200 ml of toluene. The extracted toluene solution was washed 3 times with 200 ml of a 10% aqueous sodium hydroxide solution and 5 times with 150 ml of deionized water. By dehydrating the washed toluene solution with potassium carbonate, and then distilling off the toluene under reduced pressure,
Compound A which is an allyl ether compound of the above compound a
Was obtained. The viscosity of this compound A was 50 centipoise (cP) at 25 degreeC.

As the inorganic filler, fused silica, hollow silica balloon and methyl silicate were used. The content of particles having a particle size of 20 μm or more is 4 with respect to the total amount of fused silica.
The content of particles having a particle size of 20 μm or less at 0 volume% and 60% by volume is referred to as fused silica C, and the content of particles having a particle size of 20 μm or more is 20 volume% with respect to the total amount of fused silica. The content of particles having a diameter of 20 μm or less is set to 80% by volume is referred to as fused silica D, and the content of particles having a particle size of 20 μm or more is 10 volume% and the particle size is 20 μm or less with respect to the total amount of fused silica. The fused silica E having a content of 90% by volume was referred to as fused silica E. Specific gravity of fused silica is 2.20
Met. As a hollow silica balloon, the content of particles having a particle size of 20 μm or more is 30% by volume and the content of particles having a particle size of 20 μm or less is 70 with respect to the total amount of the hollow silica balloon.
Hollow silica balloon (H-
330: manufactured by Nippon Silica Co., Ltd.) was used. As a methyl silicate, the particle size is 20μ with respect to the total amount of methyl silicate.
Methyl silicate (MSP-150: manufactured by Nikko Fine Products, Inc.) having a content of particles of m or more of 50% by volume, a content of particles of 20 μm or less of particle diameter of 50% by volume, and a specific gravity of 1.330 was used.

As a curing accelerator, 1,8 diaza-bicyclo- (5,4,0) undecene-7 [DBU] octylate salt (SA102: manufactured by San-Apro) was used.

The respective amounts shown in Table 1 were mixed based on the amounts shown in parts by weight, and the mixture was mixed at room temperature (25
A liquid epoxy resin composition was obtained by kneading with a three-roll ceramic roll at about (° C.). However, in Example 10, a kneaded product obtained by kneading a compounded product of a liquid epoxy resin composition containing an epoxy resin, a curing agent, fused silica and the like,
Add the above hollow silica balloon afterwards and use a stirrer to
The mixture was rotated at 00 rpm for 10 minutes to obtain a liquid epoxy resin composition.

Regarding Examples 1 to 15, the viscosities of these liquid epoxy resin compositions at 30 ° C. were measured by using a rotational viscometer, and cast between two glass plates at 160 ° C. for 3 hours. Each cured product was obtained by heating. These cured products are treated with 121 ° C and 2 atm PCT
The treatment was performed for 1000 hours under the conditions, and the properties of the treated product were observed. After the PCT treatment for 1000 hours, the one that was dissolved and had a tackiness was disapproved, and the one in which no abnormality was observed was regarded as good. Also, a 5 × 10 mm glass epoxy laminate (R-
(1739: manufactured by Matsushita Electric Works, Ltd.), a liquid epoxy resin composition having a thickness of 1 mm is evenly coated on the entire surface, and the temperature is 160 ° C. in a dryer.
And heat-treated for 3 hours to obtain a cured product. The maximum amount of warpage was detected by measuring the back surface of the laminate of these cured products with a surface roughness meter. The results are shown in Table 1. The composition of the inorganic filler is shown in Table 1. In addition, the low specific gravity filler in Table 1 represents the filler having a specific gravity of 0.7 to 1.5.

[0040]

[Table 1]

(Comparative Examples 1 to 7) Comparative Examples 1 to 4 were the same as Example 1 except that the respective blending amounts shown in Table 2 were used in the proportions expressed in parts by weight. hand,
After obtaining the epoxy resin composition and the cured product, the viscosity of the epoxy resin composition at 30 ° C. was measured, and the cured product was subjected to PCT treatment. Table 2 shows the results. For Comparative Example 4, phenol novolac (PSM) was used as a curing agent.
6200: manufactured by Gunei Chemical Co., Ltd.). Comparative Examples 5 to 7
In the same manner as in Example 1, except that the fused silica C of Example 1 was replaced by crystalline silica having a specific gravity of 2.60, alumina having a specific gravity of 3.90, and calcium carbonate having a specific gravity of 2.7, respectively. Then, an epoxy resin composition and a cured product were obtained, and the maximum warpage amount was detected. Table 2 shows the results.

[0042]

[Table 2]

From the results shown in Tables 1 and 2 above, the epoxy resin compositions of Examples 1 to 15 were compared with those of Comparative Examples 1 to 15.
Compared to Comparative Example 7, it has a lower viscosity and better handleability, is suitable for forming a resin sealing layer by spot sealing, maintains a stable cured product even under the severe conditions of PCT treatment, and has moisture resistance. And a highly reliable cured product excellent in heat resistance and the like, and the maximum amount of warpage of the cured product of the liquid epoxy resin composition is in Comparative Examples 1 to 1.
It was confirmed that the liquid epoxy resin composition was smaller than that of Comparative Example 7 and could give a cured product with a small amount of warpage.

Particularly, in the tenth embodiment, the maximum warp amount is 15
It was 0 μm, and it was confirmed that the liquid epoxy resin composition was capable of giving a cured product with a very small amount of warpage.

[0045]

Since the liquid epoxy resin compositions according to claims 1 to 6 of the present invention are configured as described above, the liquid epoxy resin compositions according to claims 1 to 6 of the present invention. According to the above, the viscosity is low, the handleability is good, the resin sealing layer is suitable for forming by spot sealing, the warpage is small,
It is possible to obtain a liquid epoxy resin composition capable of providing a highly reliable cured product having excellent moisture resistance and heat resistance.

Since the method for producing a liquid epoxy resin composition according to claim 7 of the present invention is constituted as described above,
According to the method for producing a liquid epoxy resin composition according to the seventh aspect of the present invention, a liquid epoxy resin composition that can give a cured product with less warp can be obtained.

Since the method for curing the liquid epoxy resin composition according to the eighth aspect of the present invention is configured as described above,
According to the method for curing a liquid epoxy resin composition according to the eighth aspect of the present invention, a cured product of a liquid epoxy resin composition having a small warp can be obtained.

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Claims (8)

[Claims] 1. A liquid epoxy resin composition which is liquid at room temperature and contains an epoxy resin, a curing agent and an inorganic filler, and a compound having a naphthalene skeleton represented by the following general formula and an acid anhydride as the curing agent. A liquid epoxy resin composition comprising the above-mentioned inorganic filler containing fused silica. Embedded image 2. A liquid epoxy resin composition which is liquid at room temperature and contains an epoxy resin, a curing agent and an inorganic filler, and a compound having a naphthalene skeleton represented by the above general formula and an aromatic amine as the curing agent. A liquid epoxy resin composition comprising the above-mentioned inorganic filler containing fused silica. 3. The liquid epoxy resin composition according to claim 1 or 2, wherein the content of the inorganic filler is 10 to 80% by weight with respect to the total amount of the liquid epoxy resin composition. Stuff. 4. The inorganic filler has particles having a particle size of 20 μm or more, a particle size of 20 μm or more, and a specific gravity of 0.
The liquid content according to any one of claims 1 to 3, wherein the content of the particles of 7 to 1.5 is 50% by volume or more with respect to the total amount of the particles having a particle diameter of 20 µm or more. Epoxy resin composition. 5. The liquid epoxy resin composition according to claim 4, wherein the inorganic filler of particles having a particle size of 20 μm or more and a specific gravity of 0.7 to 1.5 is a hollow silica balloon. . 6. The liquid epoxy resin composition according to claim 4, wherein the inorganic filler of particles having a particle size of 20 μm or more and a specific gravity of 0.7 to 1.5 is methyl silicate. 7. The hollow silica balloon is post-added to and mixed with a kneaded product obtained by kneading a compounded product of a liquid epoxy resin composition containing an epoxy resin, a curing agent and fused silica. A method for producing the liquid epoxy resin composition described. 8. A liquid epoxy resin composition, characterized in that the liquid epoxy resin composition according to any one of claims 1 to 6 is preheated at 80 to 130 ° C. and then heat treated at 150 to 200 ° C. Method.