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  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L63/00—Compositions of epoxy resins; Compositions of derivatives of epoxy resins
• • H—ELECTRICITY
  • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
  • H10W—GENERIC PACKAGES, INTERCONNECTIONS, CONNECTORS OR OTHER CONSTRUCTIONAL DETAILS OF DEVICES COVERED BY CLASS H10
  • H10W74/00—Encapsulations, e.g. protective coatings
  • H10W74/40—Encapsulations, e.g. protective coatings characterised by their materials
  • H10W74/47—Encapsulations, e.g. protective coatings characterised by their materials comprising organic materials, e.g. plastics or resins
  • H10W74/476—Organic materials comprising silicon
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  • C08L63/00—Compositions of epoxy resins; Compositions of derivatives of epoxy resins
  • C08L63/04—Epoxynovolacs
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  • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
  • C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
  • C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
  • C08G59/20—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the epoxy compounds used
  • C08G59/32—Epoxy compounds containing three or more epoxy groups
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  • C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
  • C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
  • C08G59/20—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the epoxy compounds used
  • C08G59/32—Epoxy compounds containing three or more epoxy groups
  • C08G59/3218—Carbocyclic compounds
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  • C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
  • C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
  • C08G59/40—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the curing agents used
  • C08G59/62—Alcohols or phenols
  • C08G59/621—Phenols
• • C—CHEMISTRY; METALLURGY
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  • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
  • C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
  • C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
  • C08G59/68—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the catalysts used
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  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
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  • C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
  • C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
  • C08G59/68—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the catalysts used
  • C08G59/688—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the catalysts used containing phosphorus
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
  • C08K3/00—Use of inorganic substances as compounding ingredients
  • C08K3/01—Use of inorganic substances as compounding ingredients characterized by their specific function
  • C08K3/013—Fillers, pigments or reinforcing additives
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  • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
  • C08K3/00—Use of inorganic substances as compounding ingredients
  • C08K3/34—Silicon-containing compounds
  • C08K3/36—Silica
• • C—CHEMISTRY; METALLURGY
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  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L21/00—Compositions of unspecified rubbers
• • C—CHEMISTRY; METALLURGY
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  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L51/00—Compositions of graft polymers in which the grafted component is obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers
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  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L51/00—Compositions of graft polymers in which the grafted component is obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers
  • C08L51/04—Compositions of graft polymers in which the grafted component is obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers grafted on to rubbers
• • H—ELECTRICITY
  • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
  • H10W—GENERIC PACKAGES, INTERCONNECTIONS, CONNECTORS OR OTHER CONSTRUCTIONAL DETAILS OF DEVICES COVERED BY CLASS H10
  • H10W74/00—Encapsulations, e.g. protective coatings
  • H10W74/40—Encapsulations, e.g. protective coatings characterised by their materials
  • H10W74/47—Encapsulations, e.g. protective coatings characterised by their materials comprising organic materials, e.g. plastics or resins
• • H—ELECTRICITY
  • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
  • H10W—GENERIC PACKAGES, INTERCONNECTIONS, CONNECTORS OR OTHER CONSTRUCTIONAL DETAILS OF DEVICES COVERED BY CLASS H10
  • H10W74/00—Encapsulations, e.g. protective coatings
  • H10W74/40—Encapsulations, e.g. protective coatings characterised by their materials
  • H10W74/47—Encapsulations, e.g. protective coatings characterised by their materials comprising organic materials, e.g. plastics or resins
  • H10W74/473—Encapsulations, e.g. protective coatings characterised by their materials comprising organic materials, e.g. plastics or resins containing a filler
• • C—CHEMISTRY; METALLURGY
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  • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
  • C08G2190/00—Compositions for sealing or packing joints
• • C—CHEMISTRY; METALLURGY
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  • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
  • C08K3/00—Use of inorganic substances as compounding ingredients
  • C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
  • C08K3/20—Oxides; Hydroxides
  • C08K3/22—Oxides; Hydroxides of metals
  • C08K2003/2217—Oxides; Hydroxides of metals of magnesium
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  • C08K3/00—Use of inorganic substances as compounding ingredients
  • C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
  • C08K3/20—Oxides; Hydroxides
  • C08K3/22—Oxides; Hydroxides of metals
  • C08K2003/2227—Oxides; Hydroxides of metals of aluminium
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
  • C08K3/00—Use of inorganic substances as compounding ingredients
  • C08K3/28—Nitrogen-containing compounds
  • C08K2003/282—Binary compounds of nitrogen with aluminium
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
  • C08K3/00—Use of inorganic substances as compounding ingredients
  • C08K3/38—Boron-containing compounds
  • C08K2003/387—Borates
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
  • C08K2201/00—Specific properties of additives
  • C08K2201/014—Additives containing two or more different additives of the same subgroup in C08K
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
  • C08K3/00—Use of inorganic substances as compounding ingredients
  • C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
  • C08K3/24—Acids; Salts thereof
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
  • C08K3/00—Use of inorganic substances as compounding ingredients
  • C08K3/34—Silicon-containing compounds
  • C08K3/346—Clay
• • C—CHEMISTRY; METALLURGY
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  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L2203/00—Applications
  • C08L2203/20—Applications use in electrical or conductive gadgets
  • C08L2203/206—Applications use in electrical or conductive gadgets use in coating or encapsulating of electronic parts
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L2205/00—Polymer mixtures characterised by other features
  • C08L2205/22—Mixtures comprising a continuous polymer matrix in which are dispersed crosslinked particles of another polymer
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  • C08L2207/00—Properties characterising the ingredient of the composition
  • C08L2207/53—Core-shell polymer

Definitions

• the present invention relates to a sealing resin composition used for sealing electronic components.
• thermosetting resins such as epoxy resin
• resin compositions containing polyfunctional epoxy resins, novolak-type phenol resin curing agents, and inorganic fillers as main components have become the mainstream of sealing resins due to their superior heat resistance, moldability, and electrical properties.
• a semiconductor device is manufactured by bonding a chip whose main component is single-crystal silicon to a substrate whose main component is metal or plastic via a die bonding agent whose main component is epoxy resin or the like. Since the sealant is mainly composed of a filler, a large amount of stress is applied to the inside of the sealant or to the interface between the sealant and the peripheral member due to the characteristics of these constituent members, namely differences in thermal expansion and elastic modulus. occurs. Therefore, stress relaxation by absorbing or dissipating such stress is required.
• Patent Document 1 describes a method of reducing stress by using a predetermined polyfunctional phenol resin as a curing agent and adding silicone rubber particles.
• epoxy resins and silicone rubbers inherently have poor compatibility, and for example, an external impact tends to cause defects in the cured product, starting from the interface between the two. That is, although the elastic modulus of the cured product decreases in proportion to the amount of silicone rubber particles added, mechanical properties such as bending strength may also decrease.
• the present invention has been made in view of the above problems, and an object of the present invention is to provide a composition for semiconductor encapsulation that can achieve both low elasticity and high strength, and a method for producing the same.
• epoxy resin a curing agent; an inorganic filler; A sealing resin composition containing rubber particles
• an encapsulating resin composition in which a cured product of the encapsulating resin composition has a toughness index of 80 or more and 100 or less at 25°C.
• a method for producing the sealing resin composition comprising the step of mixing the masterbatch with a curing agent and an inorganic filler to obtain a resin composition.
• a semiconductor encapsulating composition capable of achieving both low elasticity and high strength, and a method for producing the same are provided.
• a description without indicating whether it is substituted or unsubstituted includes both those having no substituent and those having a substituent.
• alkyl group includes not only alkyl groups without substituents (unsubstituted alkyl groups) but also alkyl groups with substituents (substituted alkyl groups).
• organic group as used herein means an atomic group obtained by removing one or more hydrogen atoms from an organic compound, unless otherwise specified.
• a "monovalent organic group” represents an atomic group obtained by removing one hydrogen atom from an arbitrary organic compound.
• the encapsulating resin composition of the present embodiment (which may be referred to herein as a "resin composition”) comprises an epoxy resin (A), a curing agent (B), an inorganic filler (C), and a rubber Contains particles (D).
• the encapsulating resin composition of the present embodiment has a toughness index of 80 or more and 100 or less at 25°C.
• the cured product thereof Since the resin composition of the present embodiment contains the above-mentioned components, the cured product thereof has low elasticity and high strength in a highly favorable balance.
• the balance between the elastic modulus and the strength of the cured product of the resin composition can be confirmed using the value of the toughness index as an index.
• the "toughness index” is defined as a value obtained by dividing the bending elastic modulus of the cured product at 25°C by the bending strength of the cured product at 25°C and multiplying the result by 10,000.
• Toughness index flexural modulus / flexural strength x 10000
• a resin composition whose cured product has a toughness index in the range of 80 to 100 has low elasticity and high strength, so that an electronic device obtained by using it as a sealing material has excellent reliability.
• the flexural modulus at 25°C refers to the modulus of elasticity measured at 25°C in accordance with JIS6911
• the flexural strength at 25°C refers to the strength measured at 25°C in accordance with JIS6911. .
• the toughness index of the resin composition of the present embodiment can be adjusted by selecting the type of component (A), its compounding amount, and the production method of the resin composition. Each component used for the resin composition of this embodiment is demonstrated below.
• Epoxy resin (A) The encapsulating resin composition of the present embodiment contains an epoxy resin (A).
• epoxy resins general monomers, oligomers, and polymers having two or more epoxy groups in one molecule (in other words, polyfunctional) can be used.
• the epoxy resin a non-halogenated epoxy resin is particularly preferred.
• epoxy resin (A) for example, biphenyl type epoxy resin; bisphenol type epoxy resin such as bisphenol A type epoxy resin, bisphenol F type epoxy resin, tetramethylbisphenol F type epoxy resin; stilbene type epoxy resin; phenol novolac type epoxy resin.
• cresol novolac type epoxy resins etc.
• triphenolmethane type epoxy resins alkyl-modified triphenolmethane type epoxy resins, and other polyfunctional epoxy resins
• phenol aralkyl type epoxy resins having a phenylene skeleton, phenols having a biphenylene skeleton
• Phenolic aralkyl-type epoxy resins such as aralkyl-type epoxy resins
• Dihydroxynaphthalene-type epoxy resins, naphthol-type epoxy resins such as epoxy resins obtained by glycidyl-etherifying a dimer of dihydroxynaphthalene
• Triglycidyl isocyanurate monoallyl diglycidyl isocyanate triazine nucleus-containing epoxy resins such as nurate
• bridged cyclic hydrocarbon compound-modified phenolic epoxy resins such as dicyclopentadiene-modified phenolic epoxy resins.
• Epoxy resin (A) is at least one of bisphenol type epoxy resin, biphenyl type epoxy resin, novolak type epoxy resin (eg o-cresol novolak epoxy resin), phenol aralkyl type epoxy resin, and triphenolmethane type epoxy resin. It is more preferable to include A phenol aralkyl type epoxy resin having a biphenylene skeleton is particularly preferred for controlling the elastic modulus at high temperatures.
• epoxy resin (A) for example, an epoxy resin represented by the following general formula (1), an epoxy resin represented by the following general formula (2), an epoxy resin represented by the following general formula (3), and the following general formula At least one selected from the group consisting of epoxy resins represented by formula (4) and epoxy resins represented by general formula (5) below can be used.
• the epoxy resin represented by the following general formula (1) and the epoxy resin represented by the following general formula (4) are mentioned as one of the more preferable aspects.
• Ar 1 represents a phenylene group or a naphthylene group, and when Ar 1 is a naphthylene group, the glycidyl ether group may be bonded at either the ⁇ -position or the ⁇ -position.
• Ar 2 represents any one of a phenylene group, a biphenylene group and a naphthylene group.
• R a and R b each independently represent a hydrocarbon group having 1 to 10 carbon atoms.
• g is an integer of 0-5 and h is an integer of 0-8.
• n3 represents the degree of polymerization and its average value is 1-3.
• Rc's each independently represent a hydrogen atom or a hydrocarbon group having 1 to 4 carbon atoms.
• n5 represents the degree of polymerization and its average value is 0-4.
• R d and R e each independently represent a hydrogen atom or a hydrocarbon group having 1 to 4 carbon atoms.
• n6 represents the degree of polymerization and its average value is 0-4.
• R f 's each independently represent a hydrogen atom or a hydrocarbon group having 1 to 4 carbon atoms.
• n7 represents the degree of polymerization and its average value is 0-4.
• R g 's each independently represent a hydrogen atom or a hydrocarbon group having 1 to 4 carbon atoms.
• n8 represents the degree of polymerization and its average value is 0-4.
• the number molecular weight of the epoxy resin (A) is not particularly limited, and may be appropriately selected from the viewpoint of fluidity, curability, and the like. As an example, the number molecular weight is about 100-700. Further, from the viewpoint of fluidity, etc., the ICI viscosity of the epoxy resin (A) at 150° C. is preferably 0.1 to 5.0 poise.
• the encapsulating resin composition may contain only one type of epoxy resin (A), or may contain two or more types.
• the epoxy equivalent of the epoxy resin (A) is preferably 100-400 g/eq, more preferably 150-350 g/eq.
• the epoxy equivalent of the plurality of epoxy resins (A) as a whole is preferably the above numerical value.
• the lower limit of the amount of the epoxy resin (A) in the encapsulating resin composition is, for example, preferably 3% by mass or more, and 4% by mass or more, relative to the entire encapsulating resin composition. is more preferable, and 5% by mass or more is particularly preferable.
• the upper limit of the amount of the epoxy resin (A) is, for example, preferably 50% by mass or less, more preferably 30% by mass or less, and 20% by mass with respect to the entire sealing resin composition. More preferably: By setting the content of the epoxy resin (A) to the above upper limit or less, the humidity resistance reliability and reflow resistance of an electronic device such as a power device provided with a sealing material formed using the sealing resin composition is improved. can be improved.
• the curing reaction in the composition is optimized. easier.
• the epoxy equivalent and the amount of the epoxy resin it is possible to appropriately adjust the curing/flow characteristics of the composition.
• the encapsulating resin composition of the present embodiment contains a curing agent (B).
• the curing agent (B) is not particularly limited as long as it can react with the epoxy resin (A). Examples thereof include phenolic curing agents, amine curing agents, acid anhydride curing agents and mercaptan curing agents. Among these, phenol-based curing agents are preferred from the viewpoint of a balance of flame resistance, moisture resistance, electrical properties, curability, storage stability, and the like.
• Phenolic Curing Agent The phenolic curing agent is not particularly limited as long as it is commonly used in encapsulating resin compositions.
• phenols such as phenol novolak resin and cresol novolak resin, cresol, resorcinol, catechol, bisphenol A, bisphenol F, phenylphenol, aminophenol, ⁇ -naphthol, ⁇ -naphthol, dihydroxynaphthalene and other phenols and formaldehyde
• Novolak resins obtained by condensation or co-condensation of ketones under an acidic catalyst phenol aralkyl resins having a biphenylene skeleton synthesized from the above phenols and dimethoxyparaxylene or bis(methoxymethyl)biphenyl, and phenylene skeletons
• examples include phenol aralkyl resins such as phenol aralkyl resins, and phenol resins having a trisphenylmethane skeleton.
• Amine-based curing agent include aliphatic polyamines such as diethylenetriamine (DETA), triethylenetetramine (TETA) and metaxylylenediamine (MXDA), diaminodiphenylmethane (DDM) and m-phenylenediamine (MPDA). and aromatic polyamines such as diaminodiphenylsulfone (DDS), and polyamine compounds including dicyandiamide (DICY) and organic acid dihydralazide. These may be used alone or in combination of two or more.
• DETA diethylenetriamine
• TETA triethylenetetramine
• MXDA metaxylylenediamine
• DDM diaminodiphenylmethane
• MPDA m-phenylenediamine
• aromatic polyamines such as diaminodiphenylsulfone (DDS), and polyamine compounds including dicyandiamide (DICY) and organic acid dihydralazide. These may be used alone or
• Acid anhydride curing agents include alicyclic acid anhydrides such as hexahydrophthalic anhydride (HHPA), methyltetrahydrophthalic anhydride (MTHPA), and maleic anhydride, and trimellitic anhydride ( TMA), pyromellitic anhydride (PMDA), benzophenonetetracarboxylic acid (BTDA), and aromatic acid anhydrides such as phthalic anhydride. These may be used alone or in combination of two or more.
• HHPA hexahydrophthalic anhydride
• MTHPA methyltetrahydrophthalic anhydride
• TMA trimellitic anhydride
• PMDA pyromellitic anhydride
• BTDA benzophenonetetracarboxylic acid
• aromatic acid anhydrides such as phthalic anhydride.
• Mercaptan curing agents include trimethylolpropane tris (3-mercaptobutyrate) and trimethylolethane tris (3-mercaptobutyrate). These may be used alone or in combination of two or more.
• curing agents include isocyanate compounds such as isocyanate prepolymers and blocked isocyanates, and organic acids such as carboxylic acid-containing polyester resins. These may be used alone or in combination of two or more.
• the curing agent (B) two or more different types may be used in combination.
• the present embodiment includes the combined use of a phenol-based curing agent and an amine-based curing agent.
• the amount of the curing agent (B) is preferably 0.5% by mass or more, more preferably 1% by mass or more, and 1.5% by mass or more with respect to the entire encapsulating resin composition. is particularly preferred.
• the content of the curing agent (B) is preferably 9% by mass or less, more preferably 8% by mass or less, and 7% by mass or less with respect to the entire encapsulating resin composition. is particularly preferred.
• the amount of the curing agent (B) is appropriately adjusted in relation to the amount of the epoxy resin (A). Specifically, it is preferable that the so-called “molar equivalents" (molar ratio of reactive groups) are appropriately adjusted.
• the amount of the epoxy resin (A) relative to the phenolic curing agent is preferably 0.9 to 1.5, more preferably 1.0 to 1.4, still more preferably 1.0 to 1.3, particularly preferably 1.01 to 1.20.
• the encapsulating resin composition of the present embodiment contains an inorganic filler (C).
• an inorganic filler (C) include silica, alumina, titanium white, aluminum hydroxide, magnesium hydroxide, zinc borate, and silicon nitride.
• Silica is preferable as the inorganic filler (C).
• examples of silica include fused crushed silica, fused spherical silica, crystalline silica, finely divided silica, secondary aggregated silica, and the like. Among these, fused spherical silica is particularly preferred.
• Inorganic fillers (C) are usually particles.
• the shape of the particles is preferably approximately spherical.
• the average particle size of the inorganic filler (C) is not particularly limited, but is typically 1-100 ⁇ m, preferably 1-50 ⁇ m, more preferably 1-20 ⁇ m. By having an appropriate average particle size, it is possible to secure appropriate fluidity during curing.
• the average particle size of the inorganic filler (C) is determined by volume-based particle size distribution data using a laser diffraction/scattering particle size distribution analyzer (for example, a wet particle size distribution analyzer LA-950 manufactured by HORIBA, Ltd.). It can be obtained by acquiring and processing the data. Measurements are usually done dry.
• the inorganic filler (C) such as silica is previously surface-modified with a coupling agent such as a silane coupling agent (before mixing all the components to prepare the encapsulating resin composition). good. Thereby, aggregation of the inorganic filler (C) is suppressed, and better fluidity can be obtained. In addition, the affinity between the inorganic filler (C) and other components is increased, and the dispersibility of the inorganic filler (C) is improved. This is considered to contribute to improvement in the mechanical strength of the cured product and suppression of microcracks.
• the coupling agent used for the surface treatment of the inorganic filler (C) those exemplified as the coupling agent (E) described later can be used.
• aminosilanes such as ⁇ -aminopropyltriethoxysilane and ⁇ -aminopropyltrimethoxysilane are preferably used.
• a group such as an amino group
• the dispersibility of the inorganic filler (C) in the sealing resin composition is improved. can be enhanced.
• the type of coupling agent used for the surface treatment of the inorganic filler (C) or by appropriately adjusting the amount of the coupling agent the fluidity and , the strength after curing, etc. can be controlled.
• Surface treatment of the inorganic filler (C) with a coupling agent can be performed, for example, as follows.
• a known mixer such as a ribbon mixer can be used.
• the inorganic filler (C) and the coupling agent may be charged into the mixer in advance and then the blades may be rotated, or (ii) only the inorganic filler (C) may be charged first.
• the coupling agent may be added little by little into the mixer using a spray nozzle or the like while rotating the blades.
• the inside of the mixer at low humidity (for example, humidity of 50% or less).
• humidity for example, humidity of 50% or less.
• the resulting mixture is then removed from the mixer and aged to facilitate the coupling reaction.
• the aging treatment is carried out, for example, by leaving for 1 day or more (preferably 1 to 7 days) under conditions of 20 ⁇ 5° C. and 40 to 50% RH. By carrying out under such conditions, the coupling agent can be uniformly bonded to the surface of the inorganic filler (C).
• the surface-treated (coupling treatment) inorganic filler (C) is obtained by sieving to remove coarse particles.
• the resin composition for sealing may contain only 1 type of inorganic fillers (C), and may contain 2 or more types.
• the lower limit of the content of the inorganic filler (C) is preferably 50% by mass or more, more preferably 60% by mass or more, and 65% by mass or more with respect to the entire encapsulating resin composition. is more preferable.
• the upper limit of the content of the inorganic filler (C) is, for example, preferably 95% by mass or less, more preferably 93% by mass or less, and even more preferably 90% by mass or less.
• the encapsulating resin composition of the present embodiment contains rubber particles (D).
• a resin composition containing rubber particles (D) has high strength and low elastic modulus, and thus has high toughness.
• core-shell type rubber particles are preferably used because they have an excellent toughening effect.
• Core-shell type rubber particles are obtained by graft-polymerizing a polymer different from the core component on the surface of a particulate core component mainly composed of a crosslinked rubber-like polymer, thereby partially or entirely covering the surface of the particulate core component.
• a rubber particle coated with a shell component is obtained by graft-polymerizing a polymer different from the core component on the surface of a particulate core component mainly composed of a crosslinked rubber-like polymer, thereby partially or entirely covering the surface of the particulate core component.
• Examples of the core component include crosslinked rubber particles.
• Crosslinked rubber particles include diene-based rubbers, acrylic-based rubbers, and polysiloxane-based rubbers. More specific examples include butadiene rubber, acrylic rubber, silicone rubber, butyl rubber, nitrile rubber, styrene rubber, synthetic natural rubber, ethylene propylene rubber and the like.
• shell components include diene-based rubbers, acrylic-based rubbers, and polysiloxane-based rubbers. Polymers polymerized from one or more monomers selected from the group consisting of acrylic acid esters, methacrylic acid esters and aromatic vinyl compounds are preferred.
• the shell component is preferably graft-polymerized to the core component and chemically bonded to the polymer constituting the core component.
• a crosslinked rubbery polymer composed of a polymer of styrene and butadiene is used as the core component
• a polymer of methyl methacrylate, which is a methacrylic acid ester, and styrene, which is an aromatic vinyl compound is used as the shell component. It is preferable to use
• core-shell type rubber particles include, for example, "Paraloid (registered trademark)” EXL-2655 (manufactured by Kureha Chemical Industry Co., Ltd.) composed of butadiene/alkyl methacrylate/styrene copolymer, acrylic acid ester/methacrylic acid ester.
• Staphyloid consisting of copolymers AC-3355, TR-2122 (manufactured by Takeda Pharmaceutical Company Limited), "PARALOID (registered trademark)” consisting of butyl acrylate/methyl methacrylate copolymer EXL- 2611, EXL-3387 (manufactured by Rohm & Haas), and "Kane Ace (registered trademark)” MX series (manufactured by Kaneka Corporation).
• the content of the rubber particles (D) is 0.1% by mass or more with respect to the entire encapsulating resin composition, since a resin composition capable of forming a cured product having high strength and low elastic modulus can be obtained. and more preferably 0.5% by mass or more.
• the upper limit of the rubber particle content is preferably 10% by mass or less, more preferably 5% by mass or less.
• the average particle diameter of the primary particles of the rubber particles (D) is preferably in the range of 50 to 500 nm, more preferably 50 to 300 nm, since a resin composition capable of forming a cured product having high strength and low elastic modulus can be obtained. is more preferred.
• the encapsulating resin composition of the present embodiment preferably contains a coupling agent (E).
• the coupling agent (E) here is contained in the encapsulating resin composition as a single coupling agent (E).
• the aforementioned coupling agent (bonded to the inorganic filler (B)) used for the surface treatment of the inorganic filler (B) does not correspond to the coupling agent (E) here.
• Examples of the coupling agent (E) include epoxysilane, mercaptosilane, aminosilane, alkylsilane, ureidosilane, vinylsilane, various silane compounds such as methacrylsilane, titanium compounds, aluminum chelates, aluminum/zirconium compounds, and the like.
• a known coupling agent can be used. More specifically, the following can be exemplified.
• ⁇ Silane-based coupling agents vinyltrichlorosilane, vinyltrimethoxysilane, vinyltriethoxysilane, vinyltris( ⁇ -methoxyethoxy)silane, ⁇ -methacryloxypropyltrimethoxysilane, ⁇ -(3,4-epoxycyclohexyl)ethyltri Methoxysilane, ⁇ -glycidoxypropyltrimethoxysilane, ⁇ -glycidoxypropyltriethoxysilane, ⁇ -glycidoxypropylmethyldimethoxysilane, ⁇ -methacryloxypropylmethyldiethoxysilane, ⁇ -methacryloxypropyltriethoxysilane silane, vinyltriacetoxysilane, ⁇ -mercaptopropyltrimethoxysilane, ⁇ -aminopropyltriethoxysilane, ⁇ -anilinopropyltrimethoxysilane
• ⁇ Titanate-based coupling agent isopropyl triisostearoyl titanate, isopropyl tris(dioctylpyrophosphate) titanate, isopropyl tri(N-aminoethyl-aminoethyl) titanate, tetraoctylbis(ditridecylphosphite) titanate, tetra(2,2) -diallyloxymethyl-1-butyl)bis(ditridecyl)phosphite titanate, bis(dioctylpyrophosphate)oxyacetate titanate, bis(dioctylpyrophosphate)ethylene titanate, isopropyltrioctanoyltitanate, isopropyldimethacrylisostearoyltitanate, isopropyl tridodecylbenzenesulfonyl titanate, isopropyl isostearoyl di
• the encapsulating resin composition contains the coupling agent (E), it may contain only one type of coupling agent (E), or may contain two or more types of coupling agents (E).
• the content of the coupling agent (E) is preferably 0.1% by mass or more, more preferably 0.15% by mass or more, relative to the entire encapsulating resin composition. By setting the content of the coupling agent (E) to the above lower limit or more, the dispersibility of the inorganic filler can be improved.
• the content of the coupling agent (E) is preferably 1% by mass or less, more preferably 0.5% by mass or less, relative to the entire encapsulating resin composition. By setting the content of the coupling agent (E) to the above upper limit or less, it is possible to improve the flowability of the encapsulating resin composition during encapsulation molding, and to improve the filling property and moldability.
• the encapsulating resin composition may contain a curing accelerator (F).
• the curing accelerator (F) should just accelerate the reaction (typically a cross-linking reaction) between the epoxy resin (A) and the curing agent (B).
• Examples of the curing accelerator (F) include phosphorus atom-containing compounds such as organic phosphines, tetrasubstituted phosphonium compounds, phosphobetaine compounds, adducts of phosphine compounds and quinone compounds, and adducts of phosphonium compounds and silane compounds; , 8-diazabicyclo[5.4.0]-7-undecene, benzyldimethylamine, 2-methylimidazole, etc.
• Amidine, tertiary amines, and nitrogen atom-containing compounds such as quaternary salts of amidines and amines. can include one type or two or more types.
• a phosphorus atom-containing compound from the viewpoint of improving the curability of the resin composition.
• tetrasubstituted phosphonium compounds, phosphobetaine compounds, adducts of phosphine compounds and quinone compounds, adducts of phosphonium compounds and silane compounds, etc. have latent properties. It is more preferable to include
• organic phosphines examples include primary phosphines such as ethylphosphine and phenylphosphine; secondary phosphines such as dimethylphosphine and diphenylphosphine; and tertiary phosphines such as trimethylphosphine, triethylphosphine, tributylphosphine and triphenylphosphine.
• Examples of tetra-substituted phosphonium compounds include compounds represented by the following general formula (6).
• P represents a phosphorus atom.
• R 4 , R 5 , R 6 and R 7 each independently represent an aromatic group or an alkyl group.
• A represents an anion of an aromatic organic acid having at least one functional group selected from a hydroxyl group, a carboxyl group and a thiol group on an aromatic ring.
• AH represents an aromatic organic acid having at least one functional group selected from a hydroxyl group, a carboxyl group and a thiol group on an aromatic ring.
• x and y are 1 to 3
• z is 0 to 3
• x y.
• a compound represented by the general formula (6) is obtained, for example, as follows. First, a tetra-substituted phosphonium halide, an aromatic organic acid and a base are mixed in an organic solvent and uniformly mixed to generate an aromatic organic acid anion in the solution system. Water is then added to precipitate the compound represented by general formula (6).
• R 4 , R 5 , R 6 and R 7 bonded to the phosphorus atom are phenyl groups
• AH is a compound having a hydroxyl group in the aromatic ring, that is, a phenol.
• A is preferably the anion of the phenol.
• phenols examples include monocyclic phenols such as phenol, cresol, resorcin and catechol; condensed polycyclic phenols such as naphthol, dihydroxynaphthalene and anthraquinol; bisphenols such as bisphenol A, bisphenol F and bisphenol S; Examples include polycyclic phenols such as phenylphenol and biphenol.
• Examples of phosphobetaine compounds include compounds represented by the following general formula (7).
• P represents a phosphorus atom.
• R 8 represents an alkyl group having 1 to 3 carbon atoms, and R 9 represents a hydroxyl group.
• f is 0-5 and g is 0-3.
• a compound represented by the general formula (7) is obtained, for example, as follows. First, the triaromatic-substituted phosphine, which is the third phosphine, is brought into contact with a diazonium salt to substitute the diazonium group of the triaromatic-substituted phosphine with the diazonium salt.
• Examples of adducts of phosphine compounds and quinone compounds include compounds represented by the following general formula (8).
• P represents a phosphorus atom.
• R 10 , R 11 and R 12 each represent an alkyl group having 1 to 12 carbon atoms or an aryl group having 6 to 12 carbon atoms and may be the same or different.
• R 13 , R 14 and R 15 each represent a hydrogen atom or a hydrocarbon group having 1 to 12 carbon atoms and may be the same or different, and R 14 and R 15 combine to form a cyclic structure.
• the phosphine compound used for the adduct of the phosphine compound and the quinone compound includes, for example, triphenylphosphine, tris(alkylphenyl)phosphine, tris(alkoxyphenyl)phosphine, trinaphthylphosphine, tris(benzyl)phosphine and the like.
• Substituents or those in which a substituent such as an alkyl group or an alkoxyl group is present are preferred, and examples of substituents such as an alkyl group or an alkoxyl group include those having 1 to 6 carbon atoms.
• Triphenylphosphine is preferred from the viewpoint of availability.
• the quinone compound used for the adduct of the phosphine compound and the quinone compound includes benzoquinone and anthraquinones, among which p-benzoquinone is preferable from the viewpoint of storage stability.
• the adduct can be obtained by contacting and mixing in a solvent in which both the organic tertiary phosphine and the benzoquinones can be dissolved.
• a solvent in which both the organic tertiary phosphine and the benzoquinones can be dissolved.
• ketones such as acetone and methyl ethyl ketone, which have low solubility in the adduct, are preferred. However, it is not limited to this.
• Examples of adducts of phosphonium compounds and silane compounds include compounds represented by the following general formula (9).
• P represents a phosphorus atom and Si represents a silicon atom.
• R 16 , R 17 , R 18 and R 19 each represent an aromatic or heterocyclic organic group or an aliphatic group, and may be the same or different.
• R20 is an organic group that bonds with groups Y2 and Y3 .
• R21 is an organic group that bonds with groups Y4 and Y5 .
• Y2 and Y3 each represent a group formed by releasing protons from a proton-donating group, and the groups Y2 and Y3 in the same molecule combine with silicon atoms to form a chelate structure.
• Y4 and Y5 represent a group formed by releasing protons from a proton-donating group, and the groups Y4 and Y5 in the same molecule bind to silicon atoms to form a chelate structure.
• R 20 and R 21 may be the same or different, and Y 2 , Y 3 , Y 4 and Y 5 may be the same or different.
• Z1 is an organic group having an aromatic or heterocyclic ring, or an aliphatic group.
• R 16 , R 17 , R 18 and R 19 are, for example, phenyl group, methylphenyl group, methoxyphenyl group, hydroxyphenyl group, naphthyl group, hydroxynaphthyl group, benzyl group and methyl group. , ethyl group, n-butyl group, n-octyl group and cyclohexyl group. , an aromatic group having a substituent such as a hydroxyl group or an unsubstituted aromatic group is more preferable.
• R20 is an organic group that bonds with Y2 and Y3 .
• R 21 is an organic group that bonds with groups Y 4 and Y 5 .
• Y2 and Y3 are groups formed by proton-releasing proton-donating groups, and the groups Y2 and Y3 in the same molecule bond with silicon atoms to form a chelate structure.
• Y4 and Y5 are groups in which proton-donating groups release protons, and groups Y4 and Y5 in the same molecule bond with silicon atoms to form a chelate structure.
• the groups R 20 and R 21 may be the same or different, and the groups Y 2 , Y 3 , Y 4 and Y 5 may be the same or different.
• the proton donor releases two protons
• the proton donor is preferably an organic acid having at least two carboxyl groups or hydroxyl groups in the molecule, and furthermore, the adjacent carbon atoms constituting the aromatic ring have a carboxyl group or a hydroxyl group.
• An aromatic compound having at least two hydroxyl groups is preferable, and an aromatic compound having at least two hydroxyl groups on adjacent carbon atoms constituting an aromatic ring is more preferable.
• examples include alcohol, 1,2-cyclohexanediol, 1,2-propanediol and glycerin, and among these, catechol, 1,2-dihydroxynaphthalene and 2,3-dihydroxynaphthalene are more preferred.
• Z 1 in general formula (9) represents an organic group or aliphatic group having an aromatic or heterocyclic ring, specific examples of which include a methyl group, an ethyl group, a propyl group, a butyl group and a hexyl group. and aliphatic hydrocarbon groups such as octyl group, aromatic hydrocarbon groups such as phenyl group, benzyl group, naphthyl group and biphenyl group, glycidyloxy groups such as glycidyloxypropyl group, mercaptopropyl group, aminopropyl group, mercapto groups, alkyl groups having amino groups, and reactive substituents such as vinyl groups. preferable.
• a method for producing an adduct of a phosphonium compound and a silane compound is, for example, as follows.
• a silane compound such as phenyltrimethoxysilane and a proton donor such as 2,3-dihydroxynaphthalene are added and dissolved in a flask containing methanol, and then a sodium methoxide-methanol solution is added dropwise with stirring at room temperature.
• a solution prepared in advance by dissolving a tetrasubstituted phosphonium halide such as tetraphenylphosphonium bromide in methanol is added dropwise thereto while stirring at room temperature, crystals are precipitated. Precipitated crystals are filtered, washed with water and dried in a vacuum to obtain an adduct of a phosphonium compound and a silane compound.
• the encapsulating resin composition may contain only one curing accelerator (F), or may contain two or more curing accelerators (F).
• the content of the curing accelerator (F) is preferably 0.01% by mass or more, more preferably 0.05% by mass or more, more preferably 0.10% by mass, based on the entire encapsulating resin composition. % by mass or more is more preferable.
• the content of the curing accelerator (F) is preferably 2.0% by mass or less, more preferably 1.5% by mass or less, relative to the entire encapsulating resin composition. It is more preferably 1.0% by mass or less.
• the encapsulating resin composition of the present embodiment may further contain various additives such as ion scavengers, flame retardants, colorants, mold release agents, low stress agents, antioxidants, heavy metal deactivators, etc. may include
• Hydrotalcite for example, can be used as an ion trapping agent (also called ion catcher, ion trapping agent, etc.).
• Bismuth oxide and yttrium oxide are also known as ion scavengers.
• ion trapping agent only one type may be used, or two or more types may be used in combination.
• an ion scavenger when used, its amount is, for example, 0.01 to 0.5% by mass, preferably 0.05 to 0.3% by mass, based on the entire encapsulating resin composition.
• Flame retardants include inorganic flame retardants (for example, hydrated metal compounds such as aluminum hydroxide, available from Sumitomo Chemical Co., Ltd., etc.), halogen flame retardants, phosphorus flame retardants, organic metal salt flame retardants, and the like. can be mentioned. When using a flame retardant, you may use only 1 type and may use 2 or more types together.
• the amount of the flame retardant is, for example, 0 to 15% by mass, preferably 0 to 10% by mass, based on the entire encapsulating resin composition.
• colorants include carbon black, red iron oxide, and titanium oxide.
• a coloring agent it can be used 1 type or in combination of 2 or more types.
• a coloring agent its amount is, for example, 0.1 to 0.8% by mass, preferably 0.2 to 0.5% by mass, based on the entire encapsulating resin composition.
• release agents include natural waxes, synthetic waxes such as montan acid esters, higher fatty acids or metal salts thereof, paraffin, polyethylene oxide, and the like. When using a release agent, only one type may be used, or two or more types may be used in combination. When a release agent is used, its amount is, for example, 0.1 to 0.8% by mass, preferably 0.2 to 0.5% by mass, based on the entire encapsulating resin composition.
• low-stress agents examples include silicone oil, silicone rubber, polyisoprene, 1,2-polybutadiene, polybutadiene such as 1,4-polybutadiene, styrene-butadiene rubber, acrylonitrile-butadiene rubber, polychloroprene, and poly(oxypropylene). , poly(oxytetramethylene) glycol, polyolefin glycol, poly- ⁇ -caprolactone and other thermoplastic elastomers, polysulfide rubber, fluororubber, and the like.
• silicone rubber, silicone oil, acrylonitrile-butadiene rubber, and the like are particularly preferred from the viewpoint of controlling the flexural modulus and shrinkage within the desired range and suppressing the warping of the resulting power device.
• the low-stress agent only one kind may be used, or two or more kinds may be used in combination.
• the amount of the low-stress agent is, for example, 0 to 5% by mass, preferably 0 to 3% by mass, based on the entire encapsulating resin composition.
• antioxidants examples include phenol antioxidants (dibutylhydroxytoluene, etc.), sulfur antioxidants (mercaptopropionic acid derivatives, etc.), phosphorus antioxidants (9,10-dihydro-9-oxa-10 -phosphaphenanthrene-10-oxide, etc.).
• antioxidants when antioxidants are used, only one kind may be used, or two or more kinds may be used in combination.
• an antioxidant when an antioxidant is used, its amount is, for example, 0 to 3% by mass, preferably 0 to 2% by mass, based on the entire encapsulating resin composition.
• heavy metal deactivators examples include ADEKA STAB CDA series (manufactured by ADEKA Corporation). When using a heavy metal deactivator, only one kind may be used, or two or more kinds may be used in combination.
• the amount of the heavy metal deactivator is, for example, 0 to 1% by mass, preferably 0 to 0.5% by mass, based on the entire encapsulating resin composition.
• Method for producing encapsulating resin composition As described above, in the encapsulating resin composition of the present embodiment, in order to make the toughness index at 25° C. of the cured product within the range of 80 or more and 100 or less, the method for producing the encapsulating resin composition (preparation method) is very important.
• the components described above are mixed with a known mixer or the like, further melt-kneaded with a kneader such as a roll, kneader or extruder, cooled and pulverized to obtain a sealing resin composition.
• a kneader such as a roll, kneader or extruder
• the properties of the encapsulating resin composition are as-ground powder or granules, tablet-molding after grinding, sieving of the ground material, centrifugal milling method, hot-cut method, and the like. It can be a granule produced by a granulation method in which the dispersity, fluidity, etc. are appropriately adjusted.
• the resin composition of this embodiment is - First, only the epoxy resin (A) and the rubber particles (D) are mixed to form a masterbatch, - Then, this masterbatch is mixed with other components (curing agent (B), inorganic filler (C)), etc.) It is preferable to manufacture by the procedure.
• the dispersibility of the rubber particles (D) in the encapsulating resin composition is highly uniformized, and the toughness index, strength and elastic modulus of the cured product are within the desired ranges. can do.
• the resin composition of the present embodiment obtained by the above method has a toughness index of 80 or more and 100 or less at 25°C.
• the bending elastic modulus at 25° C. of the cured product of the resin composition of the present embodiment obtained by the above method is, for example, 12000 MPa or less, preferably 11000 MPa or less.
• the lower limit of the flexural modulus at 25° C. of the cured product of the resin composition of the present embodiment is, for example, 9000 MPa or more.
• the bending strength at 25° C. of the cured product of the resin composition of the present embodiment is, for example, 95 MPa or more, preferably 98 MPa or more.
• the upper limit of the bending strength at 25° C. of the cured product of the resin composition is, for example, 120 MPa or less.
• the toughness index at 260° C. of the cured product of the resin composition of the present embodiment is, for example, 100 or more and 160 or less.
• the bending elastic modulus at 260° C. of the cured product of the resin composition of the present embodiment is, for example, 3000 MPa or less, preferably 2500 MPa or less.
• the lower limit of the flexural modulus at 260° C. of the cured product of the resin composition of the present embodiment is, for example, 1000 MPa or more.
• the bending strength at 260° C. of the cured product of the resin composition of the present embodiment is, for example, 20 MPa or more, preferably 25 MPa or more.
• the upper limit of the bending strength at 260° C. of the cured product of the resin composition is, for example, 40 MPa or less.
• the resin composition of the present embodiment achieves high strength and low elasticity of the cured product, particularly at room temperature, by using the above-described components in specific amounts or by preparing by a specific method. , and as a result, high toughness is achieved.
• the resin composition of the present embodiment is suitably used for encapsulation of semiconductor devices.
• it is suitably used as a sealing material for power devices.
• Examples 1 to 6, Comparative Examples 1 to 3 (Preparation of encapsulating resin composition) The amounts (parts by weight) of each component shown in Table 1 were mixed at room temperature using a Henschel mixer to obtain a mixture. After that, the mixture was roll kneaded at 70 to 100° C. to obtain a kneaded product. The resulting kneaded product was cooled and then pulverized to obtain a sealing resin composition.
• the amount ratio (parts by mass) of each component is as shown in Table 1. Further, the details of the components listed in Table 1 are shown below.
• Epoxy resin ⁇ Epoxy resin 1: triphenol methane type epoxy resin (manufactured by Mitsubishi Chemical Corporation, 1032H60) ⁇ Epoxy resin 2: ortho cresol novolac type epoxy resin (manufactured by Nippon Kayaku Co., Ltd., EOCN-1020-55) (curing agent) ⁇ Curing agent 1: triphenol methane type phenolic resin (manufactured by Meiwa Kasei Co., Ltd., MEH-7500) ⁇ Curing agent 2: Novolac type phenolic resin (PR-HF-3 manufactured by Sumitomo Bakelite Co., Ltd.) (rubber particles) ⁇ Rubber particle 1: core shell rubber (butadiene rubber) (Mitsubishi Chemical Corporation, S-2030) ⁇ Rubber particles 2: Core-shell rubber (acrylic rubber) (manufactured by Aica Kogyo Co., Ltd., AC-3832SD) ⁇ Rubber particles 3: core-shell rubber (acrylic rubber)
• gel time The gel time of the resin composition obtained in each example was measured. The gel time was measured by measuring the time (gel time: seconds) from melting the resin composition on a hot plate heated to 120° C. to curing while kneading with a spatula.
• Toughness index flexural modulus / flexural strength x 10000
• any of the resin compositions of each example can be used as a sealing material.
• the resin compositions of the examples have a toughness index at 25° C. of the cured product within a predetermined range, low elasticity and high strength. It was intended to be compatible with

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