Epoxy resin composition, semiconductor element encapsulant, adhesive, and semiconductor device

Abstract

To provide an epoxy resin composition that supplies a cured matter excellent in heat resistance and resin strength.SOLUTION: An epoxy resin composition contains an epoxy resin, an inorganic filler, and one or more types of surface treatment agents selected from organic silicon compounds represented by the following formulas (1) and (2).SELECTED DRAWING: None

Description

Technical Field

[0001] The present invention relates to an epoxy resin composition, a semiconductor device encapsulant, an adhesive, and a semiconductor device.

Background Art

[0002] With the miniaturization, weight reduction, and high functionality of electrical equipment, the mounting method of semiconductor chips has become mainly surface mounting from the pin insertion type. Among them, the flip chip method is a method of mounting a semiconductor chip on the wiring pattern surface of an organic substrate via a plurality of bumps, and an underfill material is filled in the gap between the organic substrate and the semiconductor chip and the gap between solder bumps. As the underfill material, a liquid resin composition containing an epoxy resin is used from the viewpoint of reliability.

[0003] In recent years, in order to process high-speed and large-capacity information, semiconductor chips have been increasing in size. As the underfill material used for the enlarged chips, low thermal expansion and high flowability are required. As a method for low thermal expansion, high filling of fillers can be mentioned, but the viscosity increases and the flowability decreases. In order to lower the viscosity, a method of lowering the viscosity by adding a reactive diluent or a solvent is used, but problems such as a decrease in heat resistance and a decrease in resin strength have arisen (Patent Document 1).

Prior Art Documents

Patent Documents

[0004]

Patent Document 1

Summary of the Invention

Problems to be Solved by the Invention

[0005] Accordingly, the present invention aims to provide an epoxy resin composition that has high fluidity and excellent workability, and further forms a cured product that has excellent adhesiveness and adhesive retention after storage at high temperature and high humidity, and also has excellent heat resistance and resin strength, and is particularly suitable as an underfill material.

Means for Solving the Problems

[0006] As a result of intensive research to solve the above problems, the present inventors have found that an epoxy resin composition containing the following (A) epoxy resin, (B) inorganic filler, and (C) surface treatment agent can solve the above problems, and have completed the present invention.

[0007] [1] (A) Epoxy resin: 100 parts by mass, (B) Inorganic filler: 20 to 1,500 parts by mass, and (C) One or more surface treatment agents selected from organosilicon compounds represented by the following formulas (1) and (2): 0.05 to 10 parts by mass An epoxy resin composition containing the above components.

Chemical Formula

Chemical Formula

Advantages of the Invention

[0008] The epoxy resin composition of the present invention has a low viscosity and excellent flowability. Further, the cured product of the epoxy resin composition of the present invention has excellent adhesiveness to substrates, particularly silicon chips, and can maintain a high adhesive force to these substrates even after storage under high temperature and high humidity conditions, and has excellent heat resistance and moisture resistance. Therefore, the epoxy resin composition of the present invention is useful as an underfill material, a semiconductor element encapsulant, or an adhesive for semiconductor devices.

Embodiments for Carrying Out the Invention

[0009] Hereinafter, the present invention will be described in detail. The epoxy resin composition of the present invention contains the following components (A) An epoxy resin, (B) An inorganic filler, and (C) A surface treatment agent which is a specific organosilicon compound and contains.

[0010] (A) Epoxy resin (A) component, the epoxy resin, is not particularly limited, and known epoxy resins can be used. For example, bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol S type epoxy resin, phenol novolac type epoxy resin, cresol novolac type epoxy resin, bisphenol A novolac type epoxy resin, bisphenol F novolac type epoxy resin, stilbene type epoxy resin, triazine skeleton-containing epoxy resin, fluorene skeleton-containing epoxy resin, trisphenol methane type epoxy resin, biphenyl type epoxy resin, xylylene type epoxy resin, biphenyl aralkyl type epoxy resin, naphthalene type epoxy resin, dicyclopentadiene type epoxy resin, aminophenol type epoxy resin, alicyclic epoxy resin, etc. can be mentioned. Also, diglycidyl ether compounds of polyfunctional phenols and polycyclic aromatics such as anthracene can be mentioned. Further, phosphorus-containing epoxy resins obtained by introducing a phosphorus compound into the epoxy resin of the (A) component exemplified above can be mentioned. These may be used alone or in combination of two or more kinds.

[0011] As the (A) component, a liquid epoxy resin having a viscosity at 25°C of preferably 0.01 to 100,000 mPa·s, more preferably 0.1 to 10,000 mPa·s is preferred. This viscosity is the value measured 2 minutes after setting the sample using a cone-plate type rotational viscometer (E-type viscometer) at a measurement temperature of 25°C based on the description in JIS Z 8803:2011.

[0012] The content of the (A) component is preferably 15 to 80% by mass, more preferably 20 to 70% by mass, and still more preferably 25 to 65% by mass in the resin composition.

[0013] (B) Inorganic filler (B) component, the inorganic filler, is added to reduce the thermal expansion coefficient and improve the moisture resistance reliability of the epoxy resin composition. Examples of the inorganic filler include silicas such as fused silica, crystalline silica, cristobalite, alumina, silicon nitride, aluminum nitride, boron nitride, titanium oxide, glass fiber, magnesium oxide, and the like.

[0014] (B) component's average particle size can be selected according to the application, preferably 0.05 - 50 μm, more preferably 0.1 - 30 μm, and even more preferably 0.5 - 10 μm. This average particle size is the volume average particle size measured by the laser diffraction method. Also, the shape of (B) component can be selected according to the application, but a spherical shape is preferred. "Spherical" refers to particles with an aspect ratio of 2.0 or less, preferably 1.5 or less, and more preferably 1.25 or less. As (B) component, spherical alumina, spherical fused silica, spherical sol - gel silica, etc. are preferred. Also, the type of inorganic filler can be used alone or in combination of two or more.

[0015] (B) component's compounding amount is 20 - 1,500 parts by mass with respect to 100 parts by mass of (A) component, preferably 50 - 1,000 parts by mass.

[0016] (C) Surface treatment agent (organosilicon compound) (C) component, the surface treatment agent, is one or more selected from organosilicon compounds represented by the following formulas (1) and (2), and has the effect of quickly reacting with active hydrogens such as hydroxyl groups present on the surface of (B) inorganic filler and improving the affinity between the inorganic filler and (A) epoxy resin.

[0017]

Chemical formula

[0018]

Chemical formula

[0019] Here, in the above general formulas (1) and (2), examples of the group represented by R 1 specifically include a methyl group, an ethyl group, a propyl group, a butyl group, and the like.

[0020] In formulas (1) and (2), examples of the alkylene group having 1 to 6 carbon atoms represented by L include a methylene group, an ethylene group, a trimethylene group, a tetramethylene group, and the like.

[0021] In formula (2), R 2 is a hydrogen atom or an alkyl group having 1 to 8 carbon atoms, or a single bond and represents a group that combines with Z 2 to form a ring structure. Examples of the alkyl group having 1 to 8 carbon atoms of R 2 are the same as those exemplified for the above R 1 , but among them, a linear or branched alkyl group having 1 to 5 carbon atoms is preferable, and a methyl group or an ethyl group is more preferable. When R 2 is a single bond and is a group that combines with Z 2 to form a ring structure, R 2 , R 2 the nitrogen atom to which they are attached, and Z 2The ring structure formed thereby is a heterocyclic structure having at least one nitrogen atom. The heterocyclic structure preferably has one or more nitrogen atoms, more preferably two or more nitrogen atoms. Further, the heterocyclic structure is preferably a 5-membered or 6-membered ring structure, more preferably a 5-membered ring structure. R 2 , R 2 The nitrogen atom to which binds and Z 2 Specific examples of the ring structure formed thereby include, but are not limited to, the following ring structures.

Chemical formula

[0022] R in the above formula represents an alkyl group having 1 to 20 carbon atoms, and examples thereof include a methyl group, an ethyl group, a propyl group, an isopropyl group, a butyl group, an isobutyl group, a t-butyl group, a pentyl group, a hexyl group, a heptyl group, an octyl group, a nonyl group, a decyl group, an undecyl group, a dodecyl group and the like. R that binds to the benzotriazole ring in the above formula 3 is independently a hydrogen atom, an alkyl group having 1 to 20 carbon atoms or two adjacent R 3 form an aliphatic or aromatic condensed ring structure having 5 to 8 carbon atoms. R 3 Examples of the alkyl group having 1 to 20 carbon atoms of R include a hydrogen atom, a methyl group, an ethyl group, a propyl group, an isopropyl group, a butyl group, an isobutyl group and the like. Further, among the aliphatic rings or aromatic rings formed by two adjacent R 3 binding together to form a condensed ring with the benzotriazole ring to which they bind, examples of the aliphatic ring include a cycloheptane ring, a cyclohexane ring and the like. Note that the hydrogen atoms of these aliphatic rings may be substituted with an alkyl group or the like. Further, examples of the aromatic ring include a monocyclic benzene ring; condensed polycyclic naphthalene ring, fluorene ring, phenanthrene ring, anthracene ring and the like. Note that the hydrogen atoms of these aromatic rings may be substituted with an alkyl group or the like.

[0023] Specific examples of the benzotriazole ring structure include, but are not limited to, the following. [Chemical formula] In the above formula, the wavy line indicates the position where it is bonded to the carbonyl carbon in the above formula (1).

[0024] Z in formula (1) 1 is a hydrogen atom or an organic group having 1 to 20 carbon atoms. Z 1 Specific examples of the organic group of include an unsubstituted or substituted monovalent hydrocarbon group having 1 to 20 carbon atoms, -N=R 5 (R 5 represents an alkylidene group having 1 to 10 carbon atoms which may be substituted with an aryl group or a heteroaryl group having 6 to 20 carbon atoms). etc. are mentioned. Z 1 The organic group of may have a substituent and may contain an ether bond or an ester bond (however, excluding those containing O at the bonding end with an oxygen atom and generating an -O-O- bond). The monovalent hydrocarbon group having 1 to 20 carbon atoms may be linear, branched, or cyclic, and examples thereof include an alkyl group having 1 to 20 carbon atoms, an aryl group having 6 to 20 carbon atoms, an aralkyl group having 7 to 20 carbon atoms, and the like. Specific examples of the above alkyl group include, in addition to the groups exemplified by R 1 , n-nonyl, n-decyl, n-undecyl, n-dodecyl, n-tridecyl, n-icosyl group, and the like. Specific examples of the above aryl group include phenyl, naphthyl group, and the like. Specific examples of the above aralkyl group include benzyl, phenylethyl group, and the like. In addition, at least a part of the hydrogen atoms of these groups may be substituted with other substituents, and examples of the other substituents include a carboxyl group, a hydroxyl group, an oxo group (=O), a thioxo group (=S), and the like. In the above formula -N=R 5 wherein, R 5Examples of the C1-C10 alkylidene group which may be substituted with an aryl group or heteroaryl group having 6 to 20 carbon atoms include linear, branched, and cyclic ones. Specific examples thereof include methylidene, ethylidene, propylidene, propane-2-ylidene, butylidene, butane-2-ylidene, pentylidene, 4-methylpentane-2-ylidene, hexylidene, cyclohexylidene, heptylidene, octylidene, nonylidene, decylidene groups, and the like. Specific examples of the substituted alkylidene group include phenylmethylidene, diphenylmethylidene groups, and the like. Specific examples of the aryl group having 6 to 20 carbon atoms include the same groups as those exemplified for the monovalent hydrocarbon group above. Specific examples of the heteroaryl group having 6 to 20 carbon atoms include pyrrol-1-yl, 1H-pyrrol-2-yl, imidazol-1-yl, imidazol-2-yl, pyrazol-1-yl, pyrazol-3-yl, pyridin-2-yl, pyridin-3-yl groups, and the like. Z in formula (2) 2 is a hydrogen atom, a hydroxyl group, or an organic group having 1 to 20 carbon atoms. Z 2 Specific examples of the organic group of 1 Z include the same groups as those of the organic group of

[0025] In formulas (1) and (2), m is an integer of 1 to 3, preferably 2 or 3, and particularly preferably 3.

[0026] The blending amount of the organosilicon compound which is the surface treatment agent of component (C) is 0.05 to 10 parts by mass, preferably 0.2 to 5 parts by mass, based on 100 parts by mass of component (A).

[0027] Further, the epoxy resin composition of the present invention preferably contains a (D) aromatic amine curing agent which will be described in detail below.

[0028] (D) Aromatic amine curing agent Examples of the aromatic amine curing agent as the component (D) include aromatic diaminodiphenylmethane compounds such as 3,3'-diethyl-4,4'-diaminodiphenylmethane, 3,3',5,5'-tetramethyl-4,4'-diaminodiphenylmethane, and 3,3',5,5'-tetraethyl-4,4'-diaminodiphenylmethane; dimethylthiotoluenediamine; diethyltoluenediamine; 2,4-diaminotoluene; 1,4-diaminobenzene; and 1,3-diaminobenzene. These can be used alone or in combination of two or more.

[0029] Regarding the blending amount of the aromatic amine curing agent, the molar ratio of all amino groups in the amine curing agent to 1 mol of epoxy groups contained in the (A) epoxy resin is preferably 0.7 to 1.2, more preferably 0.7 to 1.1, and even more preferably 0.85 to 1.05.

[0030] (E) Other additives In the epoxy resin composition of the present invention, as other additives, the component (E) can be added as necessary within a range that does not impair the object and effect of the present invention. Examples of such additives include curing accelerators, flame retardants, ion trappers, antioxidants, adhesion promoters, low stress agents, and colorants.

[0031] The curing accelerator is not particularly limited as long as it can accelerate the reaction of the epoxy resin, and conventionally known ones can be used. Examples of the curing accelerator include basic organic compounds selected from tetraphenylphosphine, imidazole, and tertiary amines. Examples of tetraphenylphosphine include tetraphenylphosphine·tetraphenylborate derivatives and the like. Examples of imidazole include 2-methylimidazole, 2-ethylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2-phenyl-4-methylimidazole, 2-phenyl-4-methyl-5-hydroxymethylimidazole, 2-phenyl-4,5-dihydroxymethylimidazole, and the like. Examples of tertiary amines include triethylamine, benzyldimethylamine, α-methylbenzyldimethylamine, 1,8-diazabicyclo[5.4.0]undecene-7, and the like.

[0032] The addition amount of the curing accelerator is preferably 0 to 20 parts by mass with respect to 100 parts by mass of the component (A). If the curing accelerator is more than the upper limit value, it may interfere with the storage stability of the epoxy resin composition.

[0033] Also, as the shape of the curing accelerator, it is preferably in the form of a powder with an average particle size of 1 to 5 μm and a maximum particle size of 20 μm or less. More preferably, it has an average particle size of 2 to 5 μm and a maximum particle size of 15 μm or less. If the average particle size is smaller than the lower limit value, the specific surface area will increase, and the viscosity of the composition may increase when mixed with the composition. If the average particle size exceeds the upper limit value, the dispersion with the epoxy resin may become non-uniform, which may cause a decrease in reliability.

[0034] Also, the purity of this curing accelerator is preferably 90% or more, more preferably 93% or more. If the purity is less than 90%, there may be variations in reactivity and curability.

[0035] The flame retardant is added for the purpose of imparting flame retardancy. The flame retardant is not particularly limited, and all known ones can be used. For example, phosphazene compounds, silicone compounds, talc carrying zinc molybdate, zinc molybdate carrying zinc oxide, aluminum hydroxide, magnesium hydroxide, molybdenum oxide, etc. can be mentioned.

[0036] The ion trap agent is added for the purpose of capturing ion impurities contained in the resin composition and preventing thermal degradation and moisture absorption degradation. The ion trap agent is not particularly limited, and all known ones can be used. For example, hydrotalcites, bismuth hydroxide compounds, rare earth oxides, etc. can be mentioned.

[0037] The antioxidant is formulated for the purpose of preventing oxidative degradation when the cured product of the epoxy resin composition is stored at a high temperature. The antioxidant may generally be a known one and is not particularly limited. Among them, phenolic antioxidants, sulfur-based antioxidants, and phosphorus-based antioxidants are preferred, and phenolic antioxidants are particularly preferred. Further, the melting point of the phenolic antioxidant is preferably 80 to 250 °C, more preferably 90 to 240 °C, and particularly preferably 100 to 220 °C.

[0038] Next, the adhesion promoter is added for the purpose of improving adhesion. Examples of the adhesion promoter include hydrolyzable group-containing organosilicon compounds other than the component (C). For example, epoxy group-containing silane coupling agents such as 3-glycidoxypropyltrimethoxysilane, 3-glycidoxypropylmethyldiethoxysilane, and 3-glycidoxypropyltriethoxysilane; methacryl group-containing silane coupling agents such as 3-methacryloxypropylmethyldiethoxysilane, 3-methacryloxypropyltriethoxysilane, and 3-methacryloxypropylmethyldimethoxysilane; amino group-containing silane coupling agents such as 3-aminopropyltriethoxysilane, N-phenyl-3-aminopropyltrimethoxysilane, N-2(aminoethyl)3-aminopropylmethyldimethoxysilane, N-2(aminoethyl)3-aminopropyltrimethoxysilane, and N-2(aminoethyl)3-aminopropyltriethoxysilane; mercapto group-containing silane coupling agents such as 3-mercaptopropyltrimethoxysilane and 3-mercaptopropylmethyldimethoxysilane, etc.

[0039] The low stress agent is added for the purpose of suppressing resin cracks and reducing elasticity. Examples of this low stress agent include liquid silicone resin, liquid acrylic resin, liquid butadiene rubber, solid silicone resin, solid acrylic resin, solid butadiene rubber, etc.

[0040] Examples of the colorant include carbon black, titanium black, titanium oxide, etc. These may be used alone or in combination of two or more.

[0041] The blending amount of the component (E) varies depending on the purpose of use of the epoxy resin composition. Usually, it can be an amount of 10% by mass or less of the whole epoxy resin composition. When blending the component (E), it is preferably 5% by mass or more.

[0042] The epoxy resin composition of the present invention can be produced by mixing the components (A), (B), and (C) and, if necessary, the (D) aromatic amine curing agent and / or (E) other additives added. The method of mixing the components and the order of mixing the components are not particularly limited, and they may be mixed using a known mixing device. However, the epoxy resin composition of the present invention is preferably produced by a method having the following first mixing step and second mixing step.

[0043] [First mixing step] The first mixing step is a step of first mixing the two components (B) and (C). That is, the first mixing step is a step of mixing the component (B) and the component (C) and treating the surface of the inorganic filler of the component (B) with the organosilicon compound which is the surface treatment agent of the component (C). When mixing these two components (B) and (C), only the components (B) and (C) may be mixed. However, for the purpose of suppressing the hydrolysis of the organosilicon compound before it comes into contact with the inorganic filler and uniformly dispersing the organosilicon compound in the inorganic filler, the organosilicon compound may be diluted with an organic solvent and used.

[0044] The above organic solvent is preferably one that does not react with the components (A) and (C). Specifically, aliphatic hydrocarbons such as hexane, pentane, octane, and isooctane, aromatic hydrocarbons such as toluene and xylene, etc. can be mentioned, and they can be used as a mixed solvent of one or more of these. Among them, it is preferable to use hexane, toluene, etc. in which the water content in the solvent is small and which is easily available.

[0045] The device used in the first mixing step can be appropriately selected according to the treatment amount of the component (C) with respect to the component (B), etc. For example, a Henschel mixer, a vertical mixer, a rocking mixer, a concrete mixer, a mixco mixer, a Lodige mixer, a ball mill, etc. can be mentioned.

[0046] As the mixing conditions for the first mixing step, the temperature is preferably 10 to 50°C, more preferably 15 to 30°C. Also, the mixing time is preferably 2 to 20 minutes, more preferably 3 to 10 minutes.

[0047] Under these conditions, the surface treatment of the inorganic filler of component (B) can be carried out using the organosilicon compound of component (C). As for the specific method of this surface treatment, for example, the inorganic filler of component (B) is put into the above-mentioned mixer or the like and stirred, and the organosilicon compound of component (C) is sprayed by a one-fluid spray or a two-fluid spray. By the above method, in the first mixing step, a surface-treated inorganic filler can be obtained as a mixture of component (B) and component (C).

[0048] [Second mixing step] The second mixing step is a step of mixing the mixture (surface-treated inorganic filler) obtained in the first mixing step with component (A). In the second mixing step, in addition to the above component (A), at least one of additives such as (D) aromatic amine curing agent, (E) curing accelerator, flame retardant, ion trap agent, and stress reduction agent may be added and mixed as necessary. Each of the components (A) to (E) may be used alone or in combination of two or more.

[0049] The above method for preparing the resin mixture and the apparatus for performing mixing, stirring, and dispersion are not particularly limited. Specifically, for example, a Lyka machine equipped with a stirring and heating device, a two-roll mill, a three-roll mill, a ball mill, a planetary mixer, or a mascoloider, etc. may be mentioned, and these apparatuses may be used in appropriate combinations. By the above method, the epoxy resin composition of the present invention can be obtained in the second mixing step.

[0050] When the epoxy resin composition of the present invention is used as a semiconductor device encapsulant, it is particularly preferably liquid at 25°C. In this case, the viscosity of this liquid epoxy resin composition is 1,000 Pa·s or less, particularly 500 Pa·s or less, at 25°C measured at a rotational speed of 1 rpm using an E-type rotational viscometer by appropriately selecting the types and blending amounts of the above-described components. The lower limit is not particularly limited, but is usually 1 Pa·s or more. As described above, the liquid epoxy resin composition of the present invention has high fluidity and excellent workability, and thus can be suitably used as an underfill material, a semiconductor element encapsulant, or an adhesive used for large chips.

[0051] In addition, the molding method and molding conditions of the epoxy resin composition of the present invention can be conventional methods, but it is preferably post-cured at 150 to 180°C for 1 to 3 hours after molding and curing at 40 to 100°C. For example, it is more preferable to perform post-curing in a hot oven at 150°C for 1 hour or more. If the post-curing is less than 1 hour at 150°C, sufficient cured product properties may not be obtained.

Examples

[0052] Hereinafter, examples and comparative examples will be shown to specifically explain the present invention, but the present invention is not limited to the following examples.

[0053] [Example 1] As a first mixing step, 1,000 g of molten spherical silica (average particle size 0.6 μm) was weighed into a 5 L Henschel mixer, and while stirring at 1,500 rpm, 6 g of an organosilicon compound represented by the following formula (3) (manufactured by Shin-Etsu Chemical Co., Ltd.) was sprayed by a two-fluid spray. After spraying, the deposits on the Henschel mixer wall were scraped off with a resin spatula and stirred at 25°C and 1,500 rpm for 3 minutes.

Chemical formula

[0054] [Example 2] In Example 1, Resin Composition 2 was obtained in the same manner as in Example 1, except that the organosilicon compound used in the first mixing step was changed to the organosilicon compound represented by the following formula (4) (manufactured by Shin-Etsu Chemical Co., Ltd.). [Chemical formula]

[0055] [Example 3] In Example 1, Resin Composition 3 was obtained in the same manner as in Example 1, except that the organosilicon compound used in the first mixing step was changed to the organosilicon compound represented by the following formula (5) (manufactured by Shin-Etsu Chemical Co., Ltd.). [Chemical formula]

[0056] [Comparative Example 1] In Example 1, Resin Composition 4 was obtained in the same manner as in Example 1, except that the organosilicon compound (manufactured by Shin-Etsu Chemical Co., Ltd.) used in the first mixing step was changed to KBM-573.

[0057] [Comparative Example 2] In Example 1, Resin Composition 5 was obtained in the same manner as in Example 1, except that the organosilicon compound (manufactured by Shin-Etsu Chemical Co., Ltd.) used in the first mixing step was changed to KBM-403.

[0058] [Viscosity] In accordance with JIS Z 8803:2011, the viscosity of the epoxy resin composition at 25°C was measured. That is, at a measurement temperature of 25°C, using a cone - plate rotational viscometer, the sample was set and the viscosity after 2 minutes was measured.

[0059] [Flow time] Two glass plates of 30 mm × 50 mm were used to sandwich and fix a polyimide tape with a thickness of 30 μm to prepare a test piece with a 30 - μm gap. The test piece was heated to 120°C, and each composition of the examples and comparative examples was poured into the gap, and the time required for it to penetrate 30 mm was measured.

[0060] [Adhesive strength] On a silicon chip with a size of 10 mm × 10 mm, each epoxy resin composition of the examples and comparative examples was applied so that the adhered area was 4 mm 2 After placing the silicon chip on it, it was heated at 120°C for 1 hour and further at 165°C for 3 hours to prepare a test piece. Using this test piece, with a bond tester DAGE - SERIES - 4000PXY (manufactured by DAGE), the shear adhesive strength at 150°C was measured as an evaluation of the adhesive strength.

[0061] [Retention rate of adhesive strength after high - temperature and high - humidity storage] On a silicon chip with a size of 10 mm × 10 mm, each epoxy resin composition of the examples and comparative examples was applied so that the adhered area was 4 mm 2 After placing the silicon chip on it, it was heated at 120°C for 1 hour and further at 165°C for 3 hours to prepare a test piece. Using this test piece, with a bond tester DAGE - SERIES - 4000PXY (manufactured by DAGE), the shear adhesive strength at 150°C was measured as an evaluation of the adhesive strength. Also, the obtained test piece was stored in PCT (121°C / humidity 100% / 2 atm) for 168 hours, cooled to room temperature, and the shear adhesive strength at 150°C was measured. The retention rate of adhesive strength after high - temperature and high - humidity storage was calculated in more detail by the following formula. Retention rate of adhesive strength after high - temperature and high - humidity storage = Shear adhesive strength after storage in PCT for 168 hours / Initial value × 100 (%)

[0062]

Table 1

Claims

1. (A) Epoxy resin: 100 parts by mass, (B) Inorganic filler: 20 to 1,500 parts by mass, and (C) One or more surface treatment agents selected from the organosilicon compounds represented by the following formulas (1) and (2): 0.05 to 10 parts by mass An epoxy resin composition containing the same. 【Chemical Formula 1】 (In formula (1), R 1 independently represents an alkyl group having 1 to 8 carbon atoms, L represents an alkylene group having 1 to 6 carbon atoms, Z 1 represents a hydrogen atom or an organic group having 1 to 20 carbon atoms, and m represents an integer of 1 to 3.) 【Chemical Formula 2】 (In formula (2), R 1 independently represents an alkyl group having 1 to 8 carbon atoms, L represents an alkylene group having 1 to 6 carbon atoms, R 2 represents a hydrogen atom, an alkyl group having 1 to 8 carbon atoms, or a group capable of combining with Z 2 to form a ring structure, Z 2 represents a hydrogen atom, a hydroxyl group, or an organic group having 1 to 20 carbon atoms, and m represents an integer of 1 to 3.)

2. The epoxy resin composition according to claim 1, wherein the particle shape of the (B) inorganic filler is spherical.

3. The epoxy resin composition according to claim 1, wherein the average particle diameter of the (B) inorganic filler is 0.05 to 50 μm.

4. The epoxy resin composition according to claim 1, further comprising (D) an aromatic amine-based curing agent.

5. The epoxy resin composition according to claim 1, which is liquid at 25°C.

6. A semiconductor element encapsulant comprising the epoxy resin composition according to any one of claims 1 to 5.

7. An adhesive comprising the epoxy resin composition according to any one of claims 1 to 5.

8. A semiconductor device comprising a cured product of the epoxy resin composition according to any one of claims 1 to 5.

Images