Liquid resin composition, electronic component device, and method for manufacturing the same

The liquid resin composition with specific silica particles and epoxy resin formulation addresses the challenge of filling narrow gaps in flip-chip semiconductor devices, enhancing encapsulation and device reliability through improved fluidity and reduced viscosity.

JP7823646B2Active Publication Date: 2026-03-04RESONAC CORP
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Authority / Receiving Office
JP · JP
Patent Type
Patents
Current Assignee / Owner
Filing Date
2023-12-14
Publication Date
2026-03-04

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Abstract

To provide a liquid resin composition having excellent filling properties.SOLUTION: A liquid resin composition contains (A) an epoxy resin, (B) a curing agent, (C) first silica particles, each of which is surface-treated with a silane coupling agent having a glycidyl group, and which has an average particle size of 5 nm or more to less than 200 nm, and (D) second silica particles with an average particle size of 0.2-5 μm. The total content of the (C) first silica particles and the (D) second silica particles is 40-80 mass%. The ratio in mass between the (C) first silica particles and the (D) second silica particles ((D) second silica particles / (C) first silica particles) is 5-600.SELECTED DRAWING: None
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Description

[Technical Field]

[0001] The present invention relates to a liquid resin composition, an electronic component device, and a method for manufacturing the same. [Background technology]

[0002] In the field of element encapsulation for electronic devices such as transistors and integrated circuits (ICs), resin encapsulation has traditionally been mainstream due to its productivity and cost advantages, and various types of resin compositions have been used. Among these, epoxy resins are widely used due to their well-balanced properties, including workability, moldability, electrical properties, moisture resistance, heat resistance, mechanical properties, and adhesion to inserts. Liquid resin compositions for electronic devices are widely used as encapsulants in bare-chip-mounted semiconductor devices, such as chip-on-board (COB), chip-on-glass (COG), and tape carrier packages (TCP). Furthermore, in flip-chip semiconductor devices in which semiconductor elements are directly bump-bonded to wiring substrates made of ceramic, glass / epoxy resin, glass / imide resin, or polyimide film, liquid resin compositions for electronic devices are used as underfill materials to fill the gap between the bump-bonded semiconductor elements and the wiring substrate. These liquid resin compositions for electronic devices play an important role in protecting electronic components from temperature, humidity, external mechanical forces, and the like.

[0003] For example, in order to provide an encapsulating epoxy resin composition having excellent moisture-resistant adhesive strength and low stress, and an electronic component device having a highly reliable (moisture resistance and thermal shock resistance) element encapsulated therein, an encapsulating epoxy resin composition containing (A) a liquid epoxy resin, (B) a curing agent containing a liquid aromatic amine, (C) rubber particles, and (D) an inorganic filler, and an electronic component device having an element encapsulated with this encapsulating epoxy resin composition have been disclosed (see, for example, Patent Document 1). [Prior art documents] [Patent documents]

[0004] [Patent Document 1] Japanese Patent Application Laid-Open No. 2001-270976 Summary of the Invention [Problem to be solved by the invention]

[0005] However, with the rapid advancement of semiconductors, the bump pitch and bump height are becoming smaller as the number of bumps increases in the flip-chip method of bump connection, resulting in narrower gaps. As semiconductors become more highly integrated, chip sizes are also increasing, and underfill materials are being required to have the ability to uniformly fill large voids with narrow gaps.

[0006] One aspect of the present invention has been made in consideration of the above-mentioned conventional circumstances, and has as its object to provide a liquid resin composition having excellent filling properties, an electronic component device encapsulated therewith, and a method for manufacturing the same. [Means for solving the problem]

[0007] Specific means for achieving the above object are as follows. <1> (A) an epoxy resin; (B) a curing agent; (C) first silica particles having an average particle diameter of 5 nm or more and less than 200 nm and surface-treated with a silane coupling agent having a glycidyl group; and (D) second silica particles having an average particle diameter of 0.2 μm to 5 μm, the total proportion of the (C) first silica particles and the (D) second silica particles is 40% by mass to 80% by mass, A liquid resin composition in which the mass ratio of the (C) first silica particles to the (D) second silica particles ((D) second silica particles / (C) first silica particles) is 5 to 600. <2> The viscosity of the epoxy resin (A) at 25°C is 1000 Pa·s or less. <1> The liquid resin composition according to claim 1. <3> The (B) curing agent includes an amine-based curing agent. <1> or <2> The liquid resin composition according to claim 1. <4> Contains ion trapping agents <1> ~ <3> The liquid resin composition according to any one of the above. <5> Contains a curing accelerator <1> ~ <4> The liquid resin composition according to any one of the above. <6> Contains antioxidants <1> ~ <5> The liquid resin composition according to any one of the above. <7> The volatile content is 5% by mass or less <1> ~ <6> The liquid resin composition according to any one of the above. <8> a substrate having a circuit layer; an electronic component disposed on the substrate and electrically connected to the circuit layer; disposed in the gap between the substrate and the electronic component <1> ~ <7> a cured product of the liquid resin composition according to any one of the above items; An electronic component device comprising: <9> a substrate having a circuit layer; and an electronic component disposed on the substrate and electrically connected to the circuit layer; <1> ~ <7> 10. A method for producing an electronic component device, comprising a step of encapsulating the device using the liquid resin composition according to any one of claims 1 to 9. [Effects of the Invention]

[0008] According to one aspect of the present invention, it is possible to provide a liquid resin composition having excellent filling properties, an electronic component device sealed with the liquid resin composition, and a method for manufacturing the same. DETAILED DESCRIPTION OF THE INVENTION

[0009] Hereinafter, embodiments for carrying out the present invention will be described in detail. However, the present invention is not limited to the following embodiments. In the following embodiments, components (including element steps, etc.) are not essential unless otherwise specified. The same applies to numerical values ​​and their ranges, and do not limit the present invention. In the present disclosure, the term "process" includes not only a process that is independent of other processes, but also a process that cannot be clearly distinguished from other processes as long as the purpose of the process is achieved. In the present disclosure, numerical ranges indicated using "to" include the numerical values ​​before and after "to" as the minimum and maximum values, respectively. In the numerical ranges described in stages in this disclosure, the upper or lower limit value described in one numerical range may be replaced with the upper or lower limit value of another numerical range described in stages. Furthermore, in the numerical ranges described in this disclosure, the upper or lower limit value of that numerical range may be replaced with a value shown in the examples. In the present disclosure, each component may contain multiple substances corresponding to the component. When multiple substances corresponding to each component are present in the composition, the content or amount of each component means the total content or amount of the multiple substances present in the composition, unless otherwise specified. In the present disclosure, the composition may contain multiple types of particles corresponding to each component. When multiple types of particles corresponding to each component are present in the composition, the particle size of each component means the value for a mixture of the multiple types of particles present in the composition, unless otherwise specified. In the present disclosure, the term "layer" includes cases where the layer is formed over the entire area when the area in which the layer exists is observed, as well as cases where the layer is formed over only a portion of the area.

[0010] <Liquid resin composition> The liquid resin composition of the present disclosure comprises (A) an epoxy resin, (B) a curing agent, (C) first silica particles having an average particle size of 5 nm or more and less than 200 nm and surface-treated with a silane coupling agent having a glycidyl group, and (D) second silica particles having an average particle size of 0.2 μm to 5 μm, wherein the total proportion of the (C) first silica particles and the (D) second silica particles is 40 mass% to 80 mass%, and the mass ratio of the (C) first silica particles to the (D) second silica particles ((D) second silica particles / (C) first silica particles) is 5 to 600. The liquid resin composition of the present disclosure has excellent filling properties. The reason for this is not clear, but is presumed to be as follows. By surface-treating silica particles having an average particle size of 5 nm or more and less than 200 nm with a silane coupling agent having a glycidyl group, the wettability of the silica particles with an epoxy resin is improved. Furthermore, by combining silica particles having an average particle size of 5 nm or more and less than 200 nm with silica particles having an average particle size of 0.2 μm to 5 μm in a predetermined ratio, the fluidity of the silica particles as a whole is improved. For these reasons, the fluidity of the liquid resin composition is improved, and as a result, the viscosity of the liquid resin composition is reduced, and it is presumed that the liquid resin composition of the present disclosure has excellent filling properties.

[0011] Each component constituting the liquid resin composition will be described below. The liquid resin composition of the present disclosure contains (A) an epoxy resin, (B) a curing agent, (C) first silica particles having an average particle size of 5 nm or more and less than 200 nm and surface-treated with a silane coupling agent having a glycidyl group, and (D) second silica particles having an average particle size of 0.2 μm to 5 μm, and may contain other components as necessary.

[0012] -Epoxy resin- The liquid resin composition of the present disclosure contains an epoxy resin (A). The epoxy resin (A) imparts curability and adhesive properties to the liquid resin composition and imparts heat resistance and durability to a cured product of the liquid resin composition. The epoxy resin is preferably a liquid epoxy resin. In the present disclosure, a solid epoxy resin can also be used in combination with the liquid epoxy resin.

[0013] Liquid epoxy resin means an epoxy resin that is liquid at room temperature (25°C). Specifically, it means that the viscosity measured at 25°C using an E-type viscometer is 1000 Pa·s or less. Specifically, the viscosity is measured using an E-type viscometer, EHD model (cone angle 3°, cone diameter 28 mm), with a measurement temperature of 25°C, a sample volume of 0.7 ml, and the rotation speed set according to the expected viscosity of the sample, referring to the following, one minute after the start of measurement. (1) When the expected viscosity is 100 Pa·s to 1000 Pa·s: Rotation speed 0.5 rpm (2) When the expected viscosity is less than 100 Pa·s: Rotation speed: 5 rpm Furthermore, a solid epoxy resin means an epoxy resin that is solid at room temperature (25°C).

[0014] The type of epoxy resin is not particularly limited. Examples of the epoxy resin include naphthalene-type epoxy resins, diglycidyl ether-type epoxy resins such as bisphenol A, bisphenol F, bisphenol AD, bisphenol S, and hydrogenated bisphenol A, epoxidized novolac resins of phenols and aldehydes, such as orthocresol novolac-type epoxy resins, glycidyl ester-type epoxy resins obtained by reacting polybasic acids such as phthalic acid and dimer acid with epichlorohydrin, and glycidylamine-type epoxy resins obtained by reacting amine compounds such as diaminodiphenylmethane, isocyanuric acid, and aminophenol with epichlorohydrin. Furthermore, examples of epoxy resins include difunctional aliphatic epoxy compounds having two epoxy groups in the molecule, such as alkylene glycol diglycidyl ether, poly(alkylene glycol) diglycidyl ether, and alkenylene glycol diglycidyl ether.

[0015] From the viewpoint of viscosity adjustment, the epoxy equivalent of the epoxy resin is preferably 80 g / eq to 400 g / eq, more preferably 85 g / eq to 350 g / eq, and even more preferably 90 g / eq to 320 g / eq. The epoxy equivalent of an epoxy resin is measured by dissolving a weighed amount of epoxy resin in a solvent such as methyl ethyl ketone, adding acetic acid and a tetraethylammonium bromide acetate solution, and then subjecting the solution to potentiometric titration with a perchloric acid / acetic acid standard solution. An indicator may be used in this titration.

[0016] Commercially available epoxy resins may be used. Specific examples of commercially available epoxy resins include amine-type epoxy resin (product name: jER630) manufactured by Mitsubishi Chemical Corporation, bisphenol F-type epoxy resin (product name: YDF-8170C) manufactured by Nippon Steel & Sumikin Chemical Co., Ltd., bisphenol A-type epoxy resin (product name: YD-128) manufactured by Nippon Steel & Sumikin Chemical Co., Ltd., naphthalene-type epoxy resin (product name: HP-4032D) manufactured by DIC Corporation, and trade name "Epogose PT (general grade)" (Yokkaichi Synthetic Co., Ltd., diglycidyl ether of polytetramethylene glycol, number average molecular weight 700 to 800). The epoxy resin is not limited to these specific examples. One type of epoxy resin may be used alone, or two or more types may be used in combination. The content of the epoxy resin is not particularly limited, and for example, as a proportion of the solid content of the liquid resin composition, it is preferably 5% by mass to 30% by mass, more preferably 7% by mass to 28% by mass, and even more preferably 10% by mass to 25% by mass.

[0017] - Hardener - The liquid resin composition of the present disclosure contains a curing agent (B). The curing agent (B) may be any agent that undergoes a polymerization reaction with the epoxy resin, and may be either liquid or solid, provided that the liquid resin composition has fluidity at room temperature (25°C). Examples of the curing agent include amine-based curing agents, phenol-based curing agents, acid anhydride-based curing agents, etc. Among these, amine-based curing agents are preferred as the curing agent.

[0018] Examples of the amine-based curing agent include chain aliphatic amines, cyclic aliphatic amines, aliphatic aromatic amines, and aromatic amines. From the viewpoint of heat resistance and electrical properties, aromatic amines are preferred, and aromatic amines in which an amino group is directly bonded to an aromatic ring and one or two aromatic rings are contained in one molecule are more preferred. Specific examples of the amine curing agent include aromatic amine curing agents having one aromatic ring, such as m-phenylenediamine, 1,3-diaminotoluene, 1,4-diaminotoluene, 2,4-diaminotoluene, 3,5-diethyl-2,4-diaminotoluene, 3,5-diethyl-2,6-diaminotoluene, and 2,4-diaminoanisole; 4,4'-diaminodiphenylmethane, 4,4'-diaminodiphenylsulfone, 4,4'-methylenebis(2-ethylaniline), 3,3'-diethyl-4,4'-diaminodiphenylmethane, and 3,4'-diaminoanisole; Examples of aromatic amine curing agents include aromatic amine curing agents with two aromatic rings such as 3',5,5'-tetramethyl-4,4'-diaminodiphenylmethane and 3,3',5,5'-tetraethyl-4,4'-diaminodiphenylmethane; hydrolysis condensates of aromatic amine curing agents; aromatic amine curing agents with a polyether structure such as polytetramethylene oxide di-p-aminobenzoate and polytetramethylene oxide di-para-aminobenzoate; condensates of aromatic diamines and epichlorohydrin; and reaction products of aromatic diamines and styrene.

[0019] Commercially available amine curing agents may be used. Specific examples of commercially available amine curing agents include amine curing agent manufactured by Nippon Kayaku Co., Ltd. (product name: Kayahard-AA) and amine curing agents manufactured by Mitsubishi Chemical Corporation (product names: jER Cure (registered trademark) 113, jER Cure (registered trademark) W, etc.), but the amine curing agents are not limited to these specific examples. A single type of amine curing agent may be used alone, or two or more types may be used in combination.

[0020] Acid anhydride curing agents include phthalic anhydride, maleic anhydride, methyl himic anhydride, himic anhydride, succinic anhydride, tetrahydrophthalic anhydride, hexahydrophthalic anhydride, chlorendic anhydride, methyltetrahydrophthalic anhydride, 3-methylhexahydrophthalic anhydride, 4-methylhexahydrophthalic anhydride, trialkyltetrahydrophthalic anhydride maleic acid adduct, benzophenonetetracarboxylic anhydride, trimellitic anhydride, pyromellitic anhydride, hydrogenated methylnadic anhydride, and various cyclic acid anhydrides such as trialkyltetrahydrophthalic anhydrides having multiple alkyl groups obtained by Diels-Alder reaction from maleic anhydride and diene compounds, and dodecenyl succinic anhydride.

[0021] Examples of phenolic curing agents include novolak resins obtained by condensing or co-condensing at least one selected from the group consisting of phenolic compounds (e.g., phenol, cresol, xylenol, resorcinol, catechol, bisphenol A, and bisphenol F) and naphthol compounds (e.g., α-naphthol, β-naphthol, and dihydroxynaphthalene) with an aldehyde compound (e.g., formaldehyde, acetaldehyde, propionaldehyde, benzaldehyde, and salicylaldehyde) in the presence of an acid catalyst; phenol-aralkyl resins; biphenyl-aralkyl resins; and naphthol-aralkyl resins. The curing agent may be used alone or in combination of two or more kinds.

[0022] The ratio of the equivalent number of the functional group of the curing agent (for example, an amino group in the case of an amine-based curing agent, a phenolic hydroxyl group in the case of a phenol-based curing agent, or an acid anhydride group in the case of an acid anhydride-based curing agent) to the equivalent number of the epoxy resin (equivalent number of curing agent / equivalent number of epoxy resin) is preferably set in the range of 0.6 to 1.4, more preferably in the range of 0.7 to 1.3, and even more preferably in the range of 0.8 to 1.2.

[0023] -Inorganic filler- The liquid resin composition of the present disclosure contains, as inorganic fillers, (C) first silica particles having an average particle diameter of 5 nm or more and less than 200 nm and surface-treated with a silane coupling agent having a glycidyl group, and (D) second silica particles having an average particle diameter of 0.2 μm to 5 μm. Examples of silica particles include colloidal silica, hydrophobic silica, and spherical silica. From the viewpoints of the fluidity of the liquid resin composition and the heat resistance of the cured product of the liquid resin composition, amorphous spherical silica is preferred. As the amorphous spherical silica, amorphous spherical silica produced by a sol-gel method is also preferred in terms of particle size controllability and purity. Note that, as the silica, a composition containing silica obtained by the production method described in JP 2007-197655 A may also be used.

[0024] The total proportion of the first silica particles and the second silica particles is 40% by mass to 80% by mass, preferably 45% by mass to 75% by mass, and more preferably 50% by mass to 75% by mass. The mass ratio of the first silica particles to the second silica particles (second silica particles / first silica particles) is 5 to 600, preferably 5 to 300, more preferably 5 to 100, and even more preferably 5 to 75. The liquid resin composition of the present disclosure may contain inorganic fillers other than silica particles. Examples of such inorganic fillers include alumina, zircon, magnesium oxide, calcium silicate, calcium carbonate, potassium titanate, silicon carbide, silicon nitride, boron nitride, aluminum nitride, beryllia, and zirconia. Examples of flame-retardant inorganic fillers include aluminum hydroxide and zinc borate. The content of other inorganic fillers in the inorganic filler is preferably 10% by mass or less, more preferably 3% by mass or less, and even more preferably 1% by mass or less.

[0025] When the total content of silica particles in the liquid resin composition is the same, the use of the first silica particles in combination with the second silica particles tends to reduce the viscosity of the liquid resin composition compared to when only the second silica particles are used as an inorganic filler. Therefore, the total content of silica particles tends to be increased without increasing the viscosity of the liquid resin composition. Increasing the total content of silica particles reduces the thermal expansion coefficient of the cured product of the liquid resin composition, and as a result, the reliability of electronic component devices encapsulated with the liquid resin composition tends to be improved.

[0026] The average particle size of the first silica particles is 5 nm or more and less than 200 nm, preferably 10 nm to 100 nm, and more preferably 20 nm to 75 nm. When the average particle size of the first silica particles is 5 nm or more, the viscosity of the liquid resin composition tends not to increase and the fluidity tends not to deteriorate. When the average particle size of the first silica particles is less than 200 nm, the viscosity of the liquid resin composition tends to be reduced.

[0027] The specific surface area of ​​the first silica particles is set to 20 m from the viewpoint of fluidity. 2 / g~500m 2 / g, and 50m 2 / g~300m 2 / g is more preferred.

[0028] The first silica particles are surface-treated with a silane coupling agent having a glycidyl group. Examples of silane coupling agents having a glycidyl group include 3-glycidoxypropylmethyldimethoxysilane, 3-glycidoxypropyltrimethoxysilane, 3-glycidoxypropylmethyldiethoxysilane, and 3-glycidoxypropyltriethoxysilane. These compounds are commercially available from Shin-Etsu Chemical Co., Ltd., etc. Note that the silane coupling agents having a glycidyl group do not include silane coupling agents having an alicyclic epoxy group such as a 3,4-epoxycyclohexyl group.

[0029] The method of surface treating silica particle with the silane coupling agent that has glycidyl group is not particularly limited, and can suitably select the surface treatment method that is commonly used.For example, the method that can be mentioned is that the solution that contains the silane coupling agent that has glycidyl group is added to the slurry that contains silica particle, and then stirred, and then the silica particle that has been surface treated is separated by filtering or the like and dried, and the method that the silane coupling agent that has glycidyl group is sprayed on silica particle and dried, etc.

[0030] The amount of the silane coupling agent having a glycidyl group used for surface treatment of the first silica particles is not particularly limited, and is preferably 0.1% by mass to 5% by mass, more preferably 0.5% by mass to 3% by mass, and even more preferably 0.5% by mass to 2% by mass.

[0031] The first silica particles may be commercially available. Specific examples of commercially available first silica particles include inorganic fillers manufactured by Admatechs Co., Ltd. (product names: YA010C, YA050C, etc.) and inorganic fillers manufactured by Sakai Chemical Industry Co., Ltd. (product name: Sciqas 0.05 μm), but the first silica particles are not limited to these specific examples. The first silica particles may be used alone or in combination of two or more types.

[0032] The proportion of the first silica particles in the inorganic filler is preferably 0.3% by mass or more. Furthermore, the proportion of the first silica particles in the inorganic filler is preferably 30% by mass or less. The proportion of the first silica particles in the inorganic filler is preferably 0.3% by mass to 30% by mass, more preferably 0.5% by mass to 25% by mass, and even more preferably 1% by mass to 20% by mass. When the proportion of the first silica particles in the inorganic filler is within the above range, a bleeding-reducing effect can be exhibited, and a liquid resin composition with excellent fluidity tends to be obtained.

[0033] The second silica particles impart heat cycle resistance, moisture resistance, insulating properties, etc. to the cured product of the liquid resin composition, and reduce stress during curing of the liquid resin composition.

[0034] The average particle size of the second silica particles is 0.2 μm to 5 μm, preferably 0.2 μm to 3 μm, more preferably 0.3 μm to 2 μm, and even more preferably 0.4 μm to 1.8 μm. The specific surface area of ​​the second silica particles is set to 1 m from the viewpoint of fluidity. 2 / g~30m 2 / g, and 2m 2 / g~20m 2 / g is more preferred.

[0035] The proportion of the second silica particles in the inorganic filler is preferably 70% by mass or more, and is preferably 99.7% by mass or less, more preferably 70% by mass to 99.7% by mass, and even more preferably 75% by mass to 99.5% by mass.

[0036] The second silica particles may have an organic group derived from the production raw material. Examples of the organic group that the second silica particles may have include alkyl groups such as methyl groups and ethyl groups.

[0037] The second silica particles may be commercially available products. Specific examples of commercially available second silica particles include spherical silica (product name: SO-E2) manufactured by Admatechs Co., Ltd. and spherical silica (product name: SE2200) manufactured by Admatechs Co., Ltd., but the second silica particles are not limited to these specific examples. The second silica particles may be used alone or in combination of two or more types.

[0038] The specific surface area (BET specific surface area) of an inorganic filler can be measured from the nitrogen adsorption capacity in accordance with JIS Z 8830:2013. An AUTOSORB-1 (product name) manufactured by QUANTACHROME can be used as an evaluation device. Because moisture adsorbed on the sample surface and in the structure is thought to affect the gas adsorption capacity, it is preferable to first perform a pretreatment by heating to remove moisture before measuring the BET specific surface area. In pretreatment, a measurement cell containing 0.05 g of sample is depressurized to 10 Pa or less using a vacuum pump, heated to 110°C, and held for at least 3 hours, after which it is naturally cooled to room temperature (25°C) while maintaining the reduced pressure. After this pretreatment, measurements are performed with an evaluation temperature of 77 K and an evaluation pressure range of less than 1 in relative pressure (equilibrium pressure relative to saturated vapor pressure).

[0039] The average particle size of the inorganic filler can be measured by the following method. The inorganic filler to be measured is added to a solvent (pure water) in a range of 1% to 5% by mass together with 1% to 8% by mass of surfactant, and the mixture is vibrated in a 110W ultrasonic cleaner for 30 seconds to 5 minutes to disperse the inorganic filler. Approximately 3 mL of the dispersion is poured into a measurement cell and measured at 25°C. A laser diffraction particle size analyzer (HORIBA, Ltd., LA920) is used to measure the volumetric particle size distribution. The average particle size is calculated as the particle size (D50%) at which the cumulative total from the smallest diameter side in the volumetric particle size distribution reaches 50%.

[0040] The ratio of the average particle size of the first silica particles to the average particle size of the second silica particles (average particle size of the second silica particles / average particle size of the first silica particles) is preferably 7 to 40, more preferably 8 to 35, and even more preferably 9 to 32.

[0041] Whether the inorganic filler contains both the first silica particles and the second silica particles can be confirmed, for example, by determining the volumetric particle size distribution (frequency distribution) of the inorganic filler. Specifically, if the volumetric frequency distribution of the inorganic filler has peaks in the range of 5 nm or more and less than 200 nm and in the range of 0.2 μm to 5 μm, it can be said that the inorganic filler contains both the first silica particles and the second silica particles. However, the confirmation method is not limited to the above method. Furthermore, the method for determining the proportion of the first or second silica particles in the inorganic filler is not particularly limited. For example, the volume-based particle size distribution (frequency distribution) of the inorganic filler is determined, and the peak corresponding to the first silica particles is separated from the peak corresponding to the second silica particles at the valley between the two peaks, and the volume of the particles contained in each separated range is divided by the total volume of the inorganic filler to determine the proportion of the first or second silica particles. When the composition of the liquid resin composition is known, the proportion of the first or second silica particles in the inorganic filler can be determined from the composition of the liquid resin composition. Note that the calculation method is not limited to the above method.

[0042] -Curing accelerator- The liquid resin composition of the present disclosure may contain a curing accelerator. The type of the curing accelerator is not particularly limited, and known curing accelerators can be used. Specifically, cycloamidine compounds such as 1,8-diaza-bicyclo[5.4.0]undecene-7, 1,5-diaza-bicyclo[4.3.0]nonene, and 5,6-dibutylamino-1,8-diaza-bicyclo[5.4.0]undecene-7; cycloamidine compounds containing maleic anhydride, 1,4-benzoquinone, 2,5-toluquinone, 1,4-naphthoquinone, 2,3-dimethylbenzoquinone, 2,6-dimethylbenzoquinone, and 2,3-dimethoxy-5-methyl-1,4-benzoquinone; Compounds with intramolecular polarization formed by adding quinone compounds such as 1,4-benzoquinone, 2,3-dimethoxy-1,4-benzoquinone, and phenyl-1,4-benzoquinone, compounds with π bonds such as diazophenylmethane and phenolic resins; tertiary amine compounds such as benzyldimethylamine, triethanolamine, dimethylaminoethanol, and tris(dimethylaminomethyl)phenol; derivatives of tertiary amine compounds; 2-methylimidazole, 2-phenylimidazole, 2-phenyl-4-methylimidazole, and 2-phenyl-4-methylimidazole. Examples of the curing accelerator include imidazole compounds such as thiimidazole; derivatives of imidazole compounds; organic phosphine compounds such as tributylphosphine, methyldiphenylphosphine, triphenylphosphine, tris(4-methylphenyl)phosphine, diphenylphosphine, and phenylphosphine; phosphorus compounds having intramolecular polarization obtained by adding a compound having a π bond, such as maleic anhydride, the above-mentioned quinone compounds, diazophenylmethane, or a phenolic resin, to an organic phosphine compound; tetraphenylboron salts such as tetraphenylphosphonium tetraphenylborate, triphenylphosphine tetraphenylborate, 2-ethyl-4-methylimidazole tetraphenylborate, and N-methylmorpholine tetraphenylborate; derivatives of tetraphenylboron salts; and adducts of phosphine compounds and tetraphenylboron salts, such as triphenylphosphonium-triphenylborane and N-methylmorpholine tetraphenylphosphonium-tetraphenylborate. One type of curing accelerator may be used alone, or two or more types may be used in combination.

[0043] The content of the curing accelerator is preferably 0.1% by mass to 8% by mass based on the total amount of the epoxy resin and the curing agent.

[0044] - Ion trap agent - The liquid resin composition of the present disclosure may contain an ion trap agent. The ion trap agent that can be used in the present disclosure is not particularly limited as long as it is an ion trap agent generally used in a sealing material used for manufacturing semiconductor devices. Examples of the ion trap agent include compounds represented by the following general formula (VI-1) or the following general formula (VI-2).

[0045] Mg 1-a Al a (OH)2(CO3) a / 2 ·uH2O (VI-1) (In the general formula (VI-1), a is 0 < a ≤ 0.5, and u is a positive number.) BiO b (OH) c (NO3) d (VI-2) (In the general formula (VI-2), b is 0.9 ≤ b ≤ 1.1, c is 0.6 ≤ c ≤ 0.8, and d is 0.2 ≤ d ≤ 0.4.)

[0046] The ion trap agent is available as a commercial product. Examples of the compound represented by the general formula (VI-1) include "DHT-4A" (trade name, Kyowa Chemical Industry Co., Ltd.) which is available as a commercial product. Also, examples of the compound represented by the general formula (VI-2) include "IXE500" (trade name, Toagosei Co., Ltd.) which is available as a commercial product.

[0047] In addition, as ion trap agents other than those described above, hydrated oxides of elements selected from magnesium, aluminum, titanium, zirconium, antimony, etc. can be mentioned. The ion trap agent may be used alone or in combination of two or more.

[0048] When the liquid resin composition contains an ion trapping agent, the content of the ion trapping agent is preferably 1 part by mass or more relative to 100 parts by mass of epoxy resin from the viewpoint of realizing sufficient moisture resistance reliability. From the viewpoint of fully exerting the effects of other components, the content of the ion trapping agent is preferably 15 parts by mass or less relative to 100 parts by mass of epoxy resin, more preferably 1 to 10 parts by mass, and even more preferably 2 to 5 parts by mass.

[0049] The average particle size of the ion trapping agent is preferably 0.1 μm to 3.0 μm, and the maximum particle size is preferably 10 μm or less. The average particle size of the ion trapping agent can be measured in the same manner as in the case of the inorganic filler.

[0050] -Antioxidants- The liquid resin composition of the present disclosure may contain an antioxidant. As the antioxidant, conventionally known antioxidants can be used. Phenolic compound antioxidants include compounds having at least one alkyl group at the ortho position of the phenol nucleus, such as 2,6-di-t-butyl-4-methylphenol, n-octadecyl-3-(3,5-di-t-butyl-4-hydroxyphenyl)propionate, 2,2'-methylenebis-(4-methyl-6-t-butylphenol), 3,9-bis[2-[3-(3-t-butyl-4-hydroxy-5-methylphenyl)propionyloxy]-1,1-dimethylethyl]-2,4,8,10-tetraoxaspiro[5.5] Undecane, 4,4'-butylidenebis-(6-t-butyl-3-methylphenol), 4,4'-thiobis(6-t-butyl-3-methylphenol), tetrakis[methylene-3-(3,5-di-t-butyl-4-hydroxyphenyl)propionate]methane, 2,2-thio-diethylenebis[3-(3,5-di-t-butyl-4-hydroxyphenyl)propionate], N,N'-hexamethylenebis[3-(3,5-di-t-butyl-4-hydroxyphenyl)propionamide], isooctyl-3-(3,5-di-t-butyl-4-hydroxyphenyl)propionamide 1,3,5-trimethyl-2,4,6-tris(3,5-di-t-butyl-4-hydroxybenzyl)benzene, 4,6-bis(dodecylthiomethyl)-o-cresol, bis[3,5-di-t-butyl-4-hydroxybenzyl(ethoxy)phosphinate]calcium, 2,4-bis(octylthiomethyl)-6-methylphenol, 1,6-hexanediol-bis[3-(3,5-di-t-butyl-4-hydroxyphenyl)propionate], 6-[3-(3-t-butyl-4 -hydroxy-5-methylphenyl)propoxy]-2,4,8,10-tetra-t-butyldibenz[d,f][1,3,2]dioxaphosphepine, 2-t-butyl-6-(3-t-butyl-2-hydroxy-5-methylbenzyl)-4-methylphenyl acrylate, 2-[1-(2-hydroxy-3,5-di-t-pentylphenyl)ethyl]-4,6-di-t-pentylphenyl acrylate, 2,2'-methylenebis-(4-ethyl-6-t-butylphenol), 2,6-di-t-butyl-4-ethylphenol, 1,1,Examples include 3-tris(2-methyl-4-hydroxy-5-t-butylphenyl)butane, triethylene glycol-bis[3-(3-t-butyl-4-hydroxy-5-methylphenyl)propionate], tris(3,5-di-t-butyl-4-hydroxybenzyl)isocyanurate, diethyl[[3,5-bis(1,1-dimethylethyl)-4-hydroxyphenyl]methyl]phosphonate, 2,5,7,8-tetramethyl-2-(4',8',12'-trimethyltridecyl)chroman-6-ol, and 2,4-bis-(n-octylthio)-6-(4-hydroxy-3,5-di-t-butylanilino)-1,3,5-triazine. Organic sulfur compound antioxidants include dilauryl-3,3'-thiodipropionate, dimyristyl-3,3'-thiodipropionate, distearyl-3,3'-thiodipropionate, pentaerythrityl tetrakis(3-laurylthiopropionate), ditridecyl-3,3'-thiodipropionate, 2-mercaptobenzimidazole, 4,4'-thiobis(6-t-butyl-3-methylpropionate), 2,4-bis(octylthiomethyl)-6-methylphenol, 2,4-bis-(n-octylthio)-6-(4-hydroxy-3,5-di-t-butylanilino)-1,3,5-triazine, and the like. Examples of amine compound antioxidants include N,N'-diallyl-p-phenylenediamine, N,N'-di-sec-butyl-p-phenylenediamine, octylated diphenylamine, and 2,4-bis-(n-octylthio)-6-(4-hydroxy-3,5-di-t-butylanilino)-1,3,5-triazine. Among the amine compound antioxidants, dicyclohexylamine is commercially available as a product under the trade name D-CHA-T manufactured by New Japan Chemical Co., Ltd., and its derivatives include dicyclohexylamine ammonium nitrite, N,N-di(3-methyl-cyclohexyl)amine, N,N-di(2-methoxy-cyclohexyl)amine, and N,N-di(4-bromo-cyclohexyl)amine. Phosphorus compound antioxidants include trisnonylphenyl phosphite, triphenyl phosphite, bis[3,5-di-t-butyl-4-hydroxybenzyl(ethoxy)phosphinate]calcium, tris(2,4-di-t-butylphenyl)phosphite, 2-[[2,4,8,10-tetrakis(1,1-dimethylether)dibenzo[d,f][1,3,2]dioxaphosphepin-6-yl]oxy]-N,N-bis[2-{[2,4,8, 10-tetrakis(1,1-dimethylethyl)dibenzo[d,f][1,3,2]dioxaphosphepin-6-yl]oxy}-ethyl]ethanamine, 6-[3-(3-t-butyl-4-hydroxy-5-methylphenyl)propoxy]-2,4,8,10-tetra-t-butyldibenz[d,f][1,3,2]dioxaphosphepin, diethyl[[3,5-bis(1,1-dimethylethyl)-4-hydroxyphenyl]methyl]phosphonate, etc. The antioxidant may be used alone or in combination of two or more. Specific examples of the antioxidant include compounds containing at least one of a phosphorus atom, a sulfur atom, and an amine in addition to a phenolic hydroxyl group, but these compounds may be mentioned multiple times.

[0051] The content of the antioxidant is preferably 0.1% by mass to 10% by mass, and more preferably 0.5% by mass to 5% by mass, based on the total epoxy resin.

[0052] -Organic solvents- The liquid resin composition of the present disclosure may contain an organic solvent as needed to reduce viscosity. In particular, when a solid epoxy resin and a solid curing agent are used, it is preferable to contain an organic solvent to obtain a liquid resin composition. The organic solvent is not particularly limited and includes alcohol-based solvents such as methyl alcohol, ethyl alcohol, propyl alcohol, and butyl alcohol; ketone-based solvents such as acetone and methyl ethyl ketone; glycol ether-based solvents such as ethylene glycol ethyl ether, ethylene glycol methyl ether, ethylene glycol butyl ether, propylene glycol methyl ether, dipropylene glycol methyl ether, propylene glycol ethyl ether, and propylene glycol methyl ether acetate; lactone-based solvents such as γ-butyrolactone, δ-valerolactone, and ε-caprolactone; amide-based solvents such as dimethylacetamide and dimethylformamide; and aromatic solvents such as toluene and xylene. One type may be used alone, or two or more types may be used in combination. Among these, organic solvents with a boiling point of 170°C or higher are preferred from the viewpoint of avoiding bubble formation due to sudden evaporation when curing the liquid resin composition.

[0053] The content of volatile matter, including organic solvents, etc., is not particularly limited as long as it is to an extent that bubbles are not formed when the liquid resin composition is cured, and is preferably 5% by mass or less, more preferably 1% by mass or less, and even more preferably 0.1% by mass or less, of the total liquid resin composition. In the present disclosure, the volatile content of a liquid resin composition is calculated by heating the liquid resin composition at 180° C. for 30 minutes, based on the difference in weight before and after heating.

[0054] -Mold release agent- The liquid resin composition of the present disclosure may contain a release agent. The type of release agent is not particularly limited, and known release agents can be used. Specific examples include higher fatty acids, carnauba wax, and polyethylene wax. One type of release agent may be used alone, or two or more types may be used in combination. When the liquid resin composition contains a release agent, the content of the release agent is preferably 10% by mass or less relative to the total amount of the epoxy resin and the curing agent, and from the viewpoint of exerting its effect, it is preferably 0.5% by mass or more.

[0055] -Coloring agent- The liquid resin composition of the present disclosure may contain a colorant (for example, carbon black). The colorant may be used alone or in combination of two or more types.

[0056] When conductive particles such as carbon black are used as the colorant, the content of conductive particles having a particle diameter of 10 μm or more is preferably 1% by mass or less. When the liquid resin composition contains conductive particles, the content of the conductive particles is preferably 3% by mass or less, and more preferably 0.01% by mass to 1% by mass, based on the total amount of the epoxy resin and the curing agent.

[0057] -Rubber particles- The liquid resin composition may contain rubber particles from the viewpoint of reducing the thermal expansion of the cured product. One type of rubber particles may be used alone, or two or more types may be used in combination. Examples of suitable rubber particles include rubber particles of styrene-butadiene rubber (SBR), nitrile-butadiene rubber (NBR), butadiene rubber (BR), urethane rubber (UR), acrylic rubber (AR), etc. Among these, from the viewpoint of heat resistance and moisture resistance, rubber particles containing acrylic rubber are preferred, and core-shell type acrylic rubber particles are more preferred.

[0058] Another example of suitable rubber particles is silicone rubber particles. Examples of silicone rubber particles include silicone rubber particles crosslinked from linear polyorganosiloxanes such as polydimethylsiloxane, polymethylphenylsiloxane, and polydiphenylsiloxane; silicone rubber particles whose surfaces are coated with silicone resin; and core-shell polymer particles comprising a core of solid silicone particles obtained by emulsion polymerization or the like and a shell of an organic polymer such as an acrylic resin. The shape of these silicone rubber particles may be amorphous or spherical, and it is preferable to use spherical silicone rubber particles in order to keep the viscosity of the liquid resin composition low. Silicone rubber particles are commercially available from Dow Corning Toray Silicone Co., Ltd., Shin-Etsu Chemical Co., Ltd., and other companies.

[0059] When the liquid resin composition contains rubber particles, the average particle size of the rubber particles is preferably fine in order to uniformly modify the liquid resin composition. The average particle size of the rubber particles is preferably in the range of 0.05 μm to 10 μm, and more preferably in the range of 0.1 μm to 5 μm. When the average particle size of the rubber particles is 0.05 μm or more, the dispersibility in the liquid resin composition tends to be further improved. When the volume average particle size of the rubber particles is 10 μm or less, the stress reduction effect tends to be further improved, and the permeability and fluidity of the liquid resin composition into fine gaps are improved, which tends to reduce the occurrence of voids and unfilled portions. The average particle size of the rubber particles is measured using the same method as for the inorganic filler.

[0060] <Method for producing liquid resin composition> The liquid resin composition can be obtained, for example, by stirring, melting, mixing, dispersing, etc., (A) epoxy resin, (B) curing agent, (C) first silica particles having an average particle size of 5 nm or more and less than 200 nm and surface-treated with a silane coupling agent having a glycidyl group, (D) second silica particles having an average particle size of 0.2 μm to 5 μm, and other components used as needed, all at once or separately, while optionally applying heat treatment. The device for mixing, stirring, dispersing, etc., of these components is not particularly limited, and examples include a mortar and pestle mill equipped with a stirrer and heater, a three-roll mill, a ball mill, a planetary mixer, a bead mill, etc. The liquid resin composition can be obtained by mixing and kneading the above components using these devices, and degassing as needed. As the first silica particles, a mixture in which the first silica particles are mixed in advance with an epoxy resin may be used in order to improve the dispersibility of the first silica particles. In this case, the content of the first silica particles in the mixture is preferably 20% by mass to 70% by mass.

[0061] The viscosity of the liquid resin composition is not particularly limited. From the viewpoint of high fluidity, the viscosity is preferably 0.1 Pa·s to 50.0 Pa·s at 25°C, more preferably 1.0 Pa·s to 50.0 Pa·s, and even more preferably 10.0 Pa·s to 50.0 Pa·s. The viscosity of the liquid resin composition is measured at 25°C using an E-type viscometer (cone angle 3°, rotation speed 10 rpm).

[0062] Furthermore, when the liquid resin composition is used as an underfill material or the like, the viscosity at 110°C is preferably 0.20 Pa·s or less, and more preferably 0.15 Pa·s or less, as an indicator of the ease of filling a narrow gap of several tens to several hundreds of micrometers with the liquid resin composition at around 100°C to 120°C. The viscosity of the liquid resin composition at 110°C is measured using a rheometer AR2000 (manufactured by TA Instruments, aluminum cone 40 mm, shear rate 32.5 / sec).

[0063] Furthermore, the liquid resin composition preferably has a thixotropic index [(viscosity at 2.5 rpm) / (viscosity at 10 rpm)], which is the ratio of the viscosity at a rotation speed of 2.5 rpm to the viscosity at a rotation speed of 10 rpm, measured at 25°C using an E-type viscometer, of 0.3 to 1.5, more preferably 0.5 to 1.2. When the thixotropic index is within the above range, the filling ability tends to be further improved. The viscosity and thixotropic index of the liquid resin composition can be adjusted to a desired range by appropriately selecting the composition of the epoxy resin, the content of the inorganic filler, etc.

[0064] The conditions for curing the liquid resin composition are not particularly limited, but it is preferable to heat the composition at 80° C. to 165° C. for 1 minute to 150 minutes.

[0065] <Electronic component equipment> The electronic component device of the present disclosure includes a substrate having a circuit layer, an electronic component disposed on the substrate and electrically connected to the circuit layer, and a cured product of the liquid resin composition of the present disclosure disposed in the gap between the substrate and the electronic component. The electronic component device of the present disclosure can be obtained by encapsulating the electronic component with the liquid resin composition of the present disclosure. By encapsulating the electronic component with the liquid resin composition, the electronic component device of the present disclosure has excellent reliability.

[0066] Examples of electronic component devices include electronic component devices obtained by mounting electronic components such as active elements such as semiconductor chips, transistors, diodes, and thyristors, and passive elements such as capacitors, resistors, resistor arrays, coils, and switches on a substrate having a circuit layer, such as a lead frame, a pre-wired tape carrier, a rigid wiring board, a flexible wiring board, glass, or a silicon wafer, and then sealing necessary parts with the liquid resin composition of the present disclosure. In particular, semiconductor devices in which semiconductor elements are flip-chip bonded to wiring formed on a rigid wiring board, a flexible wiring board, or glass by bump connection are examples of devices to which the liquid resin composition of the present disclosure can be applied. Specific examples include electronic component devices such as flip-chip BGA (Ball Grid Array), LGA (Land Grid Array), and COF (Chip On Film).

[0067] The liquid resin composition of the present disclosure is suitable as an underfill material for flip chips, offering excellent reliability. The liquid resin composition of the present disclosure is particularly suitable for use in flip chip applications, not only when the bump material connecting a wiring substrate and a semiconductor element is a conventional lead-containing solder, but also when flip chip semiconductor components are made using lead-free solder, such as Sn-Ag-Cu solder. The liquid resin composition of the present disclosure tends to maintain good reliability even for flip chips bump-connected using lead-free solder, which is physically more brittle than conventional lead solder. Furthermore, the use of the liquid resin composition of the present disclosure also tends to improve reliability when mounting chip-scale packages, such as wafer-level CSPs (chip size packages), on substrates.

[0068] <Electronic component device manufacturing method> The method for manufacturing an electronic component device according to the present disclosure includes a step of encapsulating a substrate having a circuit layer and an electronic component disposed on the substrate and electrically connected to the circuit layer using the liquid resin composition according to the present disclosure. There are no particular limitations on the process of sealing a substrate having a circuit layer and an electronic component using the liquid resin composition of the present disclosure. Examples include a post-addition method in which, after connecting the electronic component to a substrate having a circuit layer, the liquid resin composition is applied to the gap between the electronic component and the substrate by utilizing capillary action, and then a curing reaction of the liquid resin composition is carried out, and a pre-application method in which the liquid resin composition of the present disclosure is first applied to the surface of at least one of the substrate having a circuit layer and the electronic component, and then, when connecting the electronic component to the substrate by thermocompression bonding, the connection of the electronic component to the substrate and the curing reaction of the liquid resin composition are carried out all at once. Examples of methods for applying the liquid resin composition include a casting method, a dispensing method, and a printing method. [Example]

[0069] The present invention will be described below based on examples, but the present invention is not limited to the following examples. In the following examples, parts and % represent parts by mass and % by mass unless otherwise specified.

[0070] (Examples 1 to 4 and Comparative Examples 1 to 8) The components were blended to obtain the compositions shown in Tables 1 and 2, and then kneaded and dispersed using a three-roll mill and a vacuum mortar and pestle mixer to prepare the liquid resin compositions of Examples 1 to 4 and Comparative Examples 1 to 8. In the tables, the blending units are parts by mass, and "-" indicates "not blended."

[0071] The materials used in preparing the liquid resin compositions and their abbreviations are listed below. (A) Epoxy resin Epoxy resin 1: Bisphenol F epoxy resin (epoxy equivalent: 160 g / eq, viscosity at 25°C: 1 Pa·s to 2 Pa·s) Epoxy resin 2: Aminophenol-type trifunctional epoxy resin (epoxy equivalent: 95 g / eq, viscosity at 25°C: 0.5 Pa·s to 1.0 Pa·s) Epoxy resin 3: Polypropylene glycol type bifunctional epoxy resin (epoxy equivalent: 315 g / eq, viscosity at 25°C: 0.04 Pa·s to 0.06 Pa·s)

[0072] (B) Hardener Hardener 1: Diethyltoluenediamine (amine equivalent: 45g / eq) Hardener 2: 4,4'-methylenebis(2-ethylaniline) (amine equivalent: 63g / eq)

[0073] (C) First silica particles Nanosilica particles 1: average particle size 50nm, treated with phenylsilane Nanosilica particles 2: average particle size 50nm, treated with 3-glycidoxypropyltrimethoxysilane Nanosilica particles 3: average particle size 20 nm, treated with 2-(3,4-epoxycyclohexyl)ethyltrimethoxysilane Nanosilica particles 4: average particle size 10 nm, treated with 2-(3,4-epoxycyclohexyl)ethyltrimethoxysilane (D) Second silica particles Microsilica particles 1: average particle size 0.5 μm Microsilica particles 2: average particle size 1.5 μm

[0074] Curing accelerator: Triphenylphosphine Colorant: Carbon black (dispersant 90%, carbon black solids 10%), average particle size 24nm Ion trapping agent: Bismuth-based ion trapping agent Antioxidant: Tetrakis[methylene-3-(3,5-di-t-butyl-4-hydroxyphenyl)propionate]methane

[0075] (1) Fluidity: Viscosity and Thixotropy Index The viscosity of the liquid resin composition at 25°C (viscosity (25°C), Pa s) was measured using an E-type viscometer (cone angle 3°, rotation speed 10 rpm). The thixotropic index at 25°C was calculated as the ratio of the viscosity at a rotation speed of 2.5 rpm to the viscosity at a rotation speed of 10 rpm [(viscosity at 2.5 rpm) / (viscosity at 10 rpm)]. The viscosity at 110°C (viscosity (110°C), Pa·s) was measured using a rheometer AR2000 (aluminum cone 40 mm, shear rate 32.5 / sec). The results obtained are shown in Table 1 or Table 2.

[0076] (filling time) A test piece was prepared by fixing a glass plate (20 mm × 30 mm × 1 mm thick) instead of a semiconductor element on a glass slide with a gap of 10 μm. This test piece was placed on a hot plate heated to 110°C, and the liquid resin composition was applied to one side of the glass plate. The time it took for the liquid resin composition to penetrate between the glass slide and the glass plate and reach the opposite side was measured. The results obtained are shown in Table 1 or Table 2.

[0077] [Table 1]

[0078] [Table 2]

[0079] In Tables 1 and 2, "silica content" means the proportion of the total of the (C) first silica particles and the (D) second silica particles, "silica ratio" means the mass ratio of the (C) first silica particles to the (D) second silica particles ((D) second silica particles / (C) first silica particles), and "particle size ratio" means the ratio of the average particle size of the (C) first silica particles to the average particle size of the (D) second silica particles ((D) second silica particles / (C) first silica particles). As is clear from Tables 1 and 2, the filling times of the liquid resin compositions of the Examples are shorter than the filling times of the liquid resin compositions of the Comparative Examples, demonstrating that the liquid resin compositions of the present disclosure have excellent filling properties.

Claims

1. (A) an epoxy resin; (B) a curing agent; (C) first silica particles having an average particle size of 10 nm to 100 nm and surface-treated with a silane coupling agent having a glycidyl group; and (D) second silica particles having an average particle size of 0.2 μm to 3 μm, the total proportion of the (C) first silica particles and the (D) second silica particles is 50% by mass to 80% by mass, a mass ratio of the (C) first silica particles to the (D) second silica particles ((D) second silica particles / (C) first silica particles) is 5 to 75; The viscosity of the epoxy resin (A) at 25°C is 1000 Pa s or less, The liquid resin composition (A) contains a bisphenol F type epoxy resin, an aminophenol type trifunctional epoxy resin, and a polypropylene glycol type difunctional epoxy resin.

2. The liquid resin composition according to claim 1, wherein the curing agent (B) comprises an amine-based curing agent.

3. The liquid resin composition according to claim 1 or 2, further comprising an ion trapping agent.

4. The liquid resin composition according to any one of claims 1 to 3, further comprising a curing accelerator.

5. The liquid resin composition according to any one of claims 1 to 4, further comprising an antioxidant.

6. The liquid resin composition according to any one of claims 1 to 5, wherein the content of volatile matter is 5% by mass or less.

7. a substrate having a circuit layer; an electronic component disposed on the substrate and electrically connected to the circuit layer; a cured product of the liquid resin composition according to any one of claims 1 to 6, which is disposed in a gap between the substrate and the electronic component; An electronic component device comprising:

8. A method for manufacturing an electronic component device, comprising a step of encapsulating a substrate having a circuit layer and an electronic component disposed on the substrate and electrically connected to the circuit layer, using the liquid resin composition according to any one of claims 1 to 6.

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