JP6048212B2 - Silicone resin composition for bonding semiconductor elements and silicon-containing cured product using the same - Google Patents

Description

  TECHNICAL FIELD The present invention relates to a silicone resin composition for adhering semiconductor elements and a silicon-containing cured product using the same. The present invention relates to a silicone resin composition for adhering semiconductor elements that is high, excellent in heat resistance and light resistance, and excellent in coating properties, and a silicon-containing cured product using the same.

  Conventionally, a conductive adhesive obtained by adding Ag powder to an epoxy resin has been used as an adhesive for optical semiconductor elements such as red and green LEDs.

  In recent years, it has become possible to manufacture blue and white LEDs, and a transparent non-conductive adhesive is required to bond them, and a non-conductive adhesive using an epoxy resin is used (for example, Patent Documents). 1). This is composed of an alicyclic epoxy resin, a silane coupling agent, an inorganic filler, and an organic tin compound.

  However, a non-conductive adhesive using an epoxy resin has good adhesion and storage stability, but the epoxy resin gradually deteriorates due to light emission of the blue or white LED itself, resulting in coloration, and the light emitted from it. Will be absorbed and the brightness of the LED will deteriorate.

  On the other hand, a non-conductive adhesive using a silicone resin has also been developed. Since the silicone resin is excellent in light resistance, the blue or white LED itself hardly deteriorates. However, since the adhesive force of silicone resin is considerably weaker than that of epoxy resin, there are problems that a wire is not attached at the time of mounting or an LED is detached. Therefore, a transparent resin having excellent light resistance and high adhesive force is required, and Patent Documents 2 to 5 have been proposed.

  The invention disclosed in Patent Document 2 is made of a silicone-modified epoxy compound, and can be said to be an adhesive having improved light resistance derived from silicone and high epoxy-derived adhesion. In such an invention, although satisfactory in terms of light resistance and high adhesiveness, the epoxy compound itself was found to be colored by a light resistance test in the same manner as the epoxy resin, and is actually shown in Comparative Example 5 as well. .

  The invention disclosed in Patent Document 3 has a viscosity of 100 Pa.s at 25 ° C. The addition reaction curable silicone resin composition has a cured product obtained by heating at 150 ° C. for 3 hours and has a type D hardness (specified in JIS K6253) of 30 degrees or more. Since it has a siloxane structure, the adhesive strength with the chip is also relatively high. However, there is no mention of the transmittance by the heat resistance test or the light resistance test, and the superiority as a non-conductive adhesive for LED cannot be found.

  The invention disclosed in Patent Document 4 is a transparent silicone resin compound containing a waxy or solid three-dimensional network organopolysiloxane resin and an organohydrogenpolysiloxane having a SiH group. It may have an epoxy structure or an aromatic ring, which is considered to be one, and a decrease in transmittance is presumed by a light resistance test. Moreover, evaluation of adhesive force important as an adhesive is also insufficient.

Furthermore, the invention disclosed in Patent Document 5 is a transparent silicone resin compound containing a prepolymer having two or more Si-H groups in one molecule, but does not contain a silane coupling agent and is inorganic. There is no regulation of the filler content, and the light resistance test and adhesive strength evaluation are insufficient.
As described above, the conventional non-conductive adhesives for LEDs have not yet sufficiently satisfied the adhesive strength, the heat resistance test, and the light transmittance test.

Japanese Patent No. 4802667 JP 2010-285563 A JP 2009-256400 A JP 2006-342200 A JP 2009-280747 A

  In view of the above circumstances, the present invention has high adhesion when a light emitting diode (LED) chip is pressed and cured, high optical transparency, excellent heat resistance and ultraviolet resistance, and excellent adhesion to semiconductor elements. An object of the present invention is to provide a silicone resin composition for an agent and a silicon-containing cured product using the same.

  As a result of intensive studies to achieve the above object, the present inventor has obtained, as component (A), a cyclic siloxane compound (a1) and an alicyclic unsaturated compound (a2) having a vinyloxy group or an allyloxy group. A silicone compound obtained by hydrosilylation, a cyclic siloxane compound having a vinyl group as the component (B), a resin component containing the hydrosilylation catalyst as the component (C), and inorganic particles of an inorganic filler as the component (D) And a part of this component (D) was substituted with hydrophobically treated inorganic particles, and this silicone resin composition exhibited an unprecedented high adhesive strength, excellent heat resistance and We found that it has ultraviolet resistance and excellent coating properties, and confirmed that silicon-containing cured products for LEDs can be obtained by heat curing using this. This has led to the completion of the present invention.

That is, according to the first invention of the present invention, a silicone compound (A) obtained by hydrosilylating a cyclic siloxane compound (a1) and an alicyclic unsaturated compound (a2) having a vinyloxy group or an allyloxy group, vinyl Silicone for semiconductor element adhesion containing a resin component comprising a cyclic siloxane compound having a group (B), a hydrosilylation catalyst (C) , and an inorganic filler (D) which is a mixture of inorganic particles (d1) and inorganic particles (d2) a resin composition, inorganic particles (d1) and inorganic particles (d2) is, silicon fluoride, magnesium oxide, aluminum oxide, silicon dioxide, zirconium oxide or one or more identical or different species selected from titanium oxide, a is, with respect to the inorganic particles (d1) is not hydrophobized inorganic particles (d2) is hydrophobic Being processed, the content of the inorganic filler (D) is 100 parts by weight of the total of components (A) and (B) component and the (C) component is 0.1 to 40 parts by weight, the inorganic particles The ratio of (d2) is 20-80 wt% of an inorganic filler (D), The silicone resin composition for semiconductor element adhesion | attachment characterized by the above-mentioned is provided.

According to a second invention of the present invention, in the first invention, the silicone compound (A) has a hydrosilyl group concentration of 1 to 10 mmol / g, and is a silicone resin for bonding semiconductor elements. A composition is provided.
According to a third invention of the present invention, there is provided a silicone resin composition for adhering a semiconductor element, characterized in that, in the first invention, the hydrosilylation catalyst (C) is a platinum-based catalyst. .
According to a fourth aspect of the present invention, in the first aspect, the inorganic filler (D) is an inorganic material having a band gap energy of 2.8 eV or more and a refractive index of 1.2 to 1.8. A silicone resin composition for adhering semiconductor elements, characterized by being particles, is provided.
According to the fifth aspect of the present invention, in the first aspect, the inorganic particles (d2) are one or more selected from alcohols having 1 to 20 carbon atoms, organic silyl compounds, organic acids, or organic amines. A silicone resin composition for bonding a semiconductor element is provided, which is hydrophobically modified with an organic material.

  On the other hand, according to the sixth invention of the present invention, there is provided a silicon-containing cured product obtained by heat-curing the silicone resin composition of any one of the first to fifth inventions.

The silicone resin composition for a semiconductor element adhesive according to the present invention is excellent in applicability to a semiconductor element, has high adhesive strength, and gives a cured product excellent in heat resistance and light resistance after heat curing. Can do. Therefore, it is particularly useful as an adhesive for LED elements and the like.
Since this composition is highly transparent, when the LED element is bonded, the light emitted on the lower surface is transmitted through the transparent adhesive and reflected by the lead frame surface, and the light can also be output to the outside, thereby increasing the external quantum efficiency. be able to. Moreover, if it is used simultaneously as LED sealing resin, since the thermal expansion coefficient and the like are the same, peeling can be prevented at the interface between the adhesive and the sealing resin.

  Hereinafter, the silicone resin composition for a semiconductor element adhesive and the silicon-containing curable composition of the present invention will be described in detail based on preferred embodiments.

1. Silicone resin composition for adhering semiconductor elements The silicone resin composition for adhering semiconductor elements of the present invention (hereinafter also referred to as a silicone resin composition or simply a resin composition) comprises a cyclic siloxane compound (a1) and a vinyloxy group or an allyloxy group. A resin component comprising a silicone compound (A) obtained by hydrosilylating the alicyclic unsaturated compound (a2) having a cyclic siloxane compound (B) having a vinyl group, a hydrosilylation catalyst (C), and inorganic particles (d1 ) And an inorganic filler (D) that is a mixture of inorganic particles (d2), and a silicone resin composition for bonding semiconductor elements,
Inorganic particles (d1) and inorganic particles (d2) is, silicon fluoride, magnesium oxide, aluminum oxide, silicon dioxide, zirconium oxide or one or more which are identical or different species selected from titanium oxide, inorganic particles ( d1) is not subjected to hydrophobic treatment, whereas inorganic particles (d2) are subjected to hydrophobic treatment, and the content of the inorganic filler (D) is (A), (B) and (C). ) The total amount of the components is 100 to 40 parts by weight, and is 0.1 to 40 parts by weight, and the proportion of the inorganic particles (d2) is 20 to 80 wt% of the inorganic filler (D).

(1) Silicone compound (A)
The silicone compound (A) in the present invention is obtained by hydrosilylating a cyclic siloxane compound (a1) and an alicyclic unsaturated compound (a2) having a vinyloxy group or an allyloxy group.

  In the cyclic siloxane compound (a1), both ends of a silane compound monomer having 1 or 2 alkyl groups having 1 to 6 carbon atoms or phenyl groups in the side chain are bonded cyclically, and two or more Si atoms are contained in one molecule. A compound having a -H group. The number of Si—O bonds in the main chain is not particularly limited, but considering the crosslinking density and productivity of the curing reaction, for example, it is 3 to 15, and preferably 4 to 10. Since the (a1) component has a cyclic main chain structure, it has excellent compatibility with the (a2) component.

Examples of the alkyl group having 1 to 6 carbon atoms include methyl, ethyl, propyl, isopropyl, butyl, isobutyl, t-butyl, amyl, isoamyl, t-amyl, hexyl and cyclohexyl groups. Of these, a methyl group, an ethyl group, and a propyl group are preferable.
The number of phenyl groups is 3 or less, preferably 1 or less per molecule, because photodegradation occurs due to double bonds.

  Specific examples of the component (a1) include 2,4,6,8-tetramethylcyclotetrasiloxane, 2,2,4,6,8-pentamethylcyclotetrasiloxane, 2,2,4,4,6, Examples include 8-hexamethylcyclotetrasiloxane, 2,4,6,8,10-pentamethylcyclopentasiloxane, 2,4,6,8,10,12-hexamethylcyclohexasiloxane. 2,4,6,8-tetramethylcyclotetrasiloxane and 2,4,6,8,10-pentamethylcyclopentasiloxane are easily available industrially and have an appropriate number of Si-H functional groups. Is preferred, and 2,4,6,8-tetramethylcyclotetrasiloxane is more preferred. The component (a1) may be used alone or in combination of two or more.

The cycloaliphatic unsaturated compound (a2) having a vinyloxy group or an allyloxy group is a compound having 1 or 2 vinyloxy groups or allyloxy groups as reactive side chains on one or two cyclohexyl rings. In _{addition, -CH 2 -O-CH = CH} 2 group as a reactive side chain, or may have a _{-CH 2 -O-CH 2 CH =} CH 2 group. The alicyclic structure portion is rigid, and the ether group portion can give flexibility to the whole molecule, and can provide heat resistance and crack resistance to the composition.

Examples of the component (a2) compound include 1,2-cyclohexanedimethanol divinyl ether, 1,3-cyclohexanedimethanol divinyl ether, 1,4-cyclohexanedimethanol divinyl ether, 1,2,4-cyclohexane trimethanol. Examples include trivinyl ether, 1,2-cyclohexanedimethanol diallyl ether, 1,3-cyclohexanedimethanol diallyl ether, 1,4-cyclohexanedimethanol diallyl ether, and 1,2,4-cyclohexanetrimethanol triallyl ether. In addition, for example, 1,2-bis (4-vinyloxycyclohexyl) propane, 1,2-bis (4-allyloxycyclohexyl) propane and the like can be mentioned.
Of these, 1,2-cyclohexanedimethanol divinyl ether, 1,3-cyclohexanedimethanol divinyl ether, 1,4-cyclohexanedimethanol divinyl ether, and 1,2,4-cyclohexanetrimethanol trivinyl ether are preferable. Cyclohexane dimethanol divinyl ether is more preferred.

As the unsaturated compound (a2), those having a vinyl side chain or a —CH ₂ —O—CH═CH ₂ group are preferable. This is because when these groups are present, there is little coloring due to heat deterioration or light deterioration. The component (a2) may be used alone or in combination of two or more.

The silicone compound of component (A) used in the present invention is obtained by hydrosilylation reaction of the above components (a1) and (a2).
The (a1) component and the (a2) component to be hydrosilylated are blended in such a ratio as to contain two or more Si—H groups in one molecule of the silicone compound of the (A) component. For example, when the number of Si—H groups in the component (a1) is X and the number of carbon-carbon double bonds having reactivity with the Si—H group in the component (a2) is Y, X: Y Is preferably 10: 1 to 8: 1. From the viewpoint of the viscosity of the silicone compound, 7: 1 to 5: 1 is more preferable, and 4: 1 to 2: 1 is most preferable.

Thereafter, the mixture of the component (a1) and the component (a2) is reacted with a hydrosilylation catalyst. The hydrosilylation catalyst is not particularly limited, and for example, a platinum catalyst, a palladium catalyst, a rhodium catalyst, or the like is used.
In the present invention, when the other component (B), and further the components (D) and (E) are blended with the silicone compound as the component (A), the amount of the hydrosilylation catalyst used here is changed to the component (a1). The amount of reaction with the component (a2) can be more than the required amount, and thereby the additional amount of the component (C): hydrosilylation catalyst described later may be reduced.

  The hydrosilylation of the component (a1) and the component (a2) is not particularly limited depending on the reaction conditions as long as the hydrosilylation catalyst is used, and conventionally known conditions can be adopted. From the point of reaction rate, it is room temperature (25 degreeC) -130 degreeC, and it is preferable to set it as 30 to 100 degreeC. The component (a1) and the component (a2) can be used after being dissolved in a solvent. Examples of the solvent include toluene, hexane, methyl isobutyl ketone, cyclopentanone, propylene glycol monomethyl ether acetate and the like.

In the present invention, the silicone compound as the component (A) preferably has a Si—H group concentration in the molecule of 1 to 100 mmol / g determined from the ratio of the integrated values of the peaks by ¹ H-NMR analysis. Within this range, the storage stability is excellent while having high curability. The concentration of Si—H groups in the molecule is more preferably 1 to 40 mmol / g, and most preferably 1 to 20 mmol / g.
In addition, as (A) component in this invention, although the commercial item based on the description of the said patent document 5 can be utilized, if the density | concentration of Si-H group remove | deviated from 1-100 mmol / g, it is sclerosis | hardenability. Is unfavorable because it may become insufficient or the storage stability may decrease.

The silicone compound of the component (A) according to the present invention preferably has a polystyrene equivalent weight average molecular weight of 50,000 to 300,000 determined by GPC measurement. Within this range, it has excellent heat resistance while having sufficient heat resistance. The weight average molecular weight is more preferably 10,000 to 250,000, and most preferably 150,000 to 200,000.
In addition, although the commercial item based on description of the said patent document 5 can be utilized as (A) component, when the weight average molecular weight removes 50,000-300,000, will heat resistance become inadequate? Handling may be reduced.

  As a result, hydrosilylation of the compound (a1) having two or more Si-H groups in one molecule and the unsaturated compound (a2) in such a ratio that two or more Si-H groups remain in one molecule. A reacted silicone compound is obtained. In addition, the number of Si-H groups which the silicone compound of (A) component has can be calculated | required from the product of the density | concentration of a Si-H group, and a weight average molecular weight.

(2) Cyclic siloxane compound having vinyl group (B)
The component (B) in the present invention is a cyclic siloxane compound containing two or more carbon-carbon double bonds having reactivity with the Si—H group of the component (A).
The number of double bonds of the cyclic siloxane compound is preferably 3 to 15, and more preferably 3 to 8 from the viewpoint of increasing the crosslinking density of the cured product. The carbon-carbon double bond having reactivity with the Si-H group essentially requires a vinyl group and may contain an alkenyl group or the like. A vinyl group (Si—CH═CH ₂ group) bonded to a silicon atom is more preferable because of high reactivity.
The component (B) has the same basic skeleton as the cyclic siloxane compound (a1), but is characterized by having a reactive double bond in the side chain.

  Specific examples of the component (B) include 2,4,6-trimethyl-2,4,6-trivinylcyclotrisiloxane, 2,4,6,6,8,8-hexamethyl-2,4-divinylcyclo Tetrasiloxane, 2,4,6,8,8-pentamethyl-2,4,6-trivinylcyclotetrasiloxane, 2,4,6,8-tetramethyl-2,4,6,8-tetravinylcyclotetra Siloxane, 2,4,6,8-tetramethyl-8-phenyl-2,4,6-trivinylcyclotetrasiloxane, 2,4,6,8-tetramethyl-6,8-diphenyl-2,4- Divinylcyclotetrasilosane, 2,4,6,8,10-pentamethyl-2,4,6,8,10-pentavinylcyclopentasiloxane, 2,4,6,8,10,12-hexamethyl-2, 4, 6, 8, 0,12- hexa vinyl cyclohexasiloxane and the like.

Among them, 2,4,6,8-tetramethyl-2-4,6,8-tetravinylcyclotetrasiloxane, 2,4,6,8-tetramethyl-8-phenyl-2,4,6-trivinylcyclo Tetrasiloxane, 2,4,6,8-tetramethyl-6,8-diphenyl-2,4-divinylcyclotetrasiloxane, 2,4,6,8,10-pentamethyl-2,4,6,8,10 -Pentavinylcyclopentasiloxane, 2,4,6,8,10,12-hexamethyl-2,4,6,8,10,12-hexavinylcyclohexasiloxane is preferred.
In view of reactivity, 2,4,6,8,10-pentamethyl-2,4,6,8,10-pentavinylcyclopentasiloxane, 2,4,6,8,10,12-hexamethyl-2,4 6,8,10,12-hexavinylcyclohexasiloxane is more preferred, and 2,4,6,8-tetramethyl-2,4,6,8-tetravinylcyclotetrasiloxane is most preferred.

  The component (B) in the present invention is a cyclic siloxane compound containing two or more carbon-carbon double bonds having reactivity with the Si—H group in one molecule, and therefore has higher heat resistance than a non-siloxane compound. The cured product has higher physical strength (rigidity) than the linear siloxane compound, and has excellent base resistance, crack resistance, and the like.

  In the composition of the present invention, the amounts of the component (A) and the component (B) are blended in consideration of the number of Si-H groups and the ratio of the number of carbon-carbon double bonds that react with the Si-H groups. To do. It is preferable that the equivalent ratio of the Si—H group and the carbon-carbon double bond having reactivity with the Si—H group is 0.9 to 10, more preferably 1.0 to 5.0, 1.1 -3.0 is most preferred. If this is shown by the mass%, 2-50 mass% of (B) component will be mix | blended with 50-98 mass% of (A) component. More preferably, 30 to 10% by mass of (B) component is blended with 70 to 90% by mass of (A) component, and 15 to 5% by mass of (B) component to 85 to 95% by mass of (A) component. It is particularly preferable to blend.

(3) Hydrosilylation catalyst (C)
The component (C) in the present invention is not particularly limited as long as it has catalytic activity for hydrosilylation reaction. Examples of such a catalyst include complexes or compounds made of Group VIII metals such as platinum, ruthenium, rhodium, palladium, osmium and indium. Preference is given to the use of platinum, palladium and rhodium catalysts used for the hydrosilylation of the cyclic siloxane compound (a1) and the alicyclic unsaturated compound (a2) having a vinyloxy group or an allyloxy group.

Examples of the platinum-based catalyst include chloroplatinic acid, complexes of chloroplatinic acid and alcohols, aldehydes, ketones, platinum-olefin complexes, platinum-carbonylvinylmethyl complexes (Ossko catalysts), platinum-divinyltetramethyldisiloxane complexes ( Karstcdt catalyst), platinum-cyclovinylmethylsiloxane complex, platinum-octylaldehyde complex, platinum-phosphine complex (for example, Pt [P (C ₆ H ₅ ) ₃ ] ₄ , PtCl [P (C ₆ H ₅ ) ₃ ] ₃ , Pt [P (OC ₄ H ₉ ) ₃ ] ₄ ), dicarbonyldichloroplatinum and the like.
Examples of the palladium-based catalyst or rhodium-based catalyst include compounds containing a palladium atom or a rhodium atom in place of the platinum atom of the platinum-based catalyst. These may be used alone or in combination of two or more. The hydrosilylation catalyst is preferably a platinum-based catalyst in terms of high reactivity, more preferably a platinum-divinyltetramethyldisiloxane complex or a platinum-carbonylvinylmethyl complex, and most preferably a platinum-carbonylvinylmethyl complex.

In the silicone resin composition of the present invention, the content of the component (C) is preferably 5% by mass or less from the viewpoint of reactivity, curability, and storage stability. In consideration of economy, 0.0001 to 1.0 mass% is more preferable, and 0.001 to 0.1 mass% is most preferable.
In the present invention, since the hydrosilylation catalyst is used when synthesizing the silicone compound of the component (A), the amount added here may be added as the component (C). In other words, if an excessive amount of hydrosilylation catalyst is used in the synthesis of the silicone compound of component (A) and the excess amount is sufficient for hydrosilylation of component (B), it is necessary to add a new one. Absent.

(4) Inorganic filler (D)
In the present invention, light transmissive inorganic particles are used as the inorganic filler of the component (D). This inorganic filler functions as a thixo modifier that adjusts the viscosity of the silicone resin composition, improves the strength of the cured product when the silicone resin composition is cured, and further adheres to LEDs or the like that are semiconductor elements. The feature is that the emitted light is not absorbed.

  In the present invention, the inorganic filler (D) is said to adhere the resin component comprising the silicone compound (A), the cyclic siloxane compound (B) having a vinyl group, and the hydrosilylation catalyst (C) to the semiconductor element substrate. It has a function.

<Inorganic particles (d1)>
Examples of such an inorganic filler include silicon fluoride, magnesium oxide, aluminum oxide, titanium oxide, zirconium oxide, and silicon dioxide. Hereinafter, one or more selected from these are referred to as inorganic particles (d1). Of these, silicon dioxide is particularly preferred. These particles (powder) can be used alone, but two or more kinds may be mixed and used.

As the inorganic filler in the present invention, it is desirable to use inorganic particles having a band gap energy of 2.8 eV or more and a refractive index of 1.2 to 1.8. This is because when the band gap energy of the inorganic particles is 2.8 eV or more, when an LED or the like, which is a semiconductor element, is bonded, light of the emitted wavelength is not absorbed by the inorganic particles. In general, wavelength absorption in an inorganic compound is mainly caused by excitation absorption of a semiconductor compound, and the band gap energy of the inorganic compound corresponds to this energy.
On the other hand, when the band gap energy is less than 2.8 eV, the wavelength absorption region of the particles becomes 440 nm or more, which causes light absorption in a light emitting LED or the like. The silicone compound (A) used in the present invention has a refractive index of about 1.4 to 1.6. Accordingly, when inorganic particles having a refractive index of 1.2 to 1.8, which is close to the refractive index, are used, light transmittance can be obtained. In particular, it is preferable to use inorganic particles having a refractive index of about 1.4 to 1.6 equivalent to the refractive index of the silicone compound (A). If the refractive index is out of the range of 1.2 to 1.8, light transmittance may not be obtained.
The color of the inorganic particles is not particularly limited, but in order to prevent light wavelength absorption, white powder or powder having the same color as the wavelength emitted by the LED or the like to which it adheres is desirable.

  For this reason, the inorganic particles are not particularly limited by the size of the particle size as long as the refractive index is within the above range. When using inorganic particles having a refractive index outside the range of 1.4 to 1.6, it is desirable that the average particle size of the primary particles be 3.0 μm or less. When the average particle size exceeds 3.0 μm, the light transmittance may be lowered depending on the type of the inorganic filler. Therefore, the average particle size of the primary particles is particularly preferably 0.8 μm or less. . If this condition is satisfied, light having a wavelength of 0.4 to 0.8 μm is not blocked, so that there is almost no influence on light transmittance. When the average particle size of the primary particles is 0.4 μm or less, and further 0.25 μm or less, the light transmittance is further improved.

The added amount of the inorganic particles is 0.1 to 40 parts by weight with respect to 100 parts by weight of the resin component comprising the component (A), the component (B) and the component (C). This is because if the addition amount is less than 0.1 parts by weight, the function as a thixotropic agent that the inorganic filler gives to the composition cannot be obtained, while if it exceeds 40 parts by weight, the thixotropy becomes high. This is because the viscosity is too high and the viscosity becomes too high, which makes it difficult to apply and reduces workability. The preferred content is 0.5 to 30 parts by weight, and further in the range of 1 to 20 parts by weight.
It is desirable that the primary particles of the inorganic filler are present dispersed in the composition. When they can aggregate to form secondary particles, it is preferable to take measures such as blending a dispersant.

  The surface of the inorganic particle (d1) is usually covered with a hydroxyl group (OH group) and is hydrophilic in relation to moisture in the atmosphere. Therefore, the viscosity is increased during use due to the influence of moisture in the atmosphere, and the coating property is adversely affected.

<Inorganic particles (d2)>
Therefore, in the present invention, the inorganic particles (D) are composed of a mixture of the inorganic particles (d1) not subjected to the hydrophobic treatment and the inorganic particles (d2) subjected to the hydrophobic treatment .
The hydrophobic treatment means that inorganic particles (d1) covered with hydroxyl groups (OH groups) and hydrophilic are reacted with organic substances that react with the OH groups, that is, alcohols having 1 to 20 carbon atoms, organic silyl compounds, organic acids. The hydrophobic modification treatment is performed with one or more selected from organic amines.

  Examples of the alcohol having 1 to 20 carbon atoms include methanol, ethanol, propanol, butanol, linear or branched pentanol, hexanol, heptanol, octanol, nonanol, decanol and the like. Preference is given to one or more of methanol, ethanol, propanol and butanol.

The organic silyl compound, for example, silica [tetraalkoxysilanes have (tetramethoxysilane, tetra C _1-4 alkoxysilane or its oligomer, such as tetraethoxysilane) and the like reactive group, unsaturated double bond backbone Alternatively, a reactive silane derivative having a terminal, a coupling agent (such as a silane coupling agent or a titanium coupling agent), or a polyorganosiloxane may be used.
As the silane coupling agent, those that generate a silanol group by hydrolysis can be used. For example, as an alkoxysilane compound, tetramethoxysilane, tetraethoxysilane, methyltrimethoxysilane, methyltriethoxysilane, dimethyldimethoxysilane, dimethyldisilane. Examples include ethoxysilane, phenyltrimethoxysilane, phenyltriethoxysilane, diphenyldimethoxysilane, diphenyldiethoxysilane, hexyltrimethoxysilane, hexyltriethoxysilane, decyltrimethoxysilane, and decyltriethoxysilane. Examples of chlorosilane include methyltrichlorosilane, dimethyldichlorosilane, trimethylchlorosilane, phenyltrichlorosilane, and diphenyldichlorosilane. Furthermore, vinyltrimethoxysilane containing vinyl group, vinyltriethoxysilane, 3-glycidoxypropyltrimethoxysilane containing epoxy group, 3-glycidoxypropyltriethoxysilane, 3-containing methacryloxy group Mention may be made of methacryloxypropyltrimethoxysilane, 3-methacryloxypropylmethyldiethoxysilane, and 3-methacryloxypropyltriethoxysilane.
Among these, for light-emitting diode (LED) chips, tetramethoxysilane, tetraethoxysilane, methyltrimethoxysilane, methyltriethoxysilane, dimethyldimethoxysilane, dimethyldiethoxy have no chlorine group or aromatic group. Alkoxysilane compounds such as silane, hexyltrimethoxysilane, hexyltriethoxysilane, decyltrimethoxysilane, and decyltriethoxysilane are preferred.

The polyorganosiloxane, for example, polydialkylsiloxane (e.g., polydiene C _1-10 alkyl siloxanes such as polydimethylsiloxane (dimethicone), preferably polydiene C _1-4 alkyl), poly alkyl alkenyl siloxane (e.g., polymethyl Poly C _1-10 alkyl C _2-10 alkenyl siloxanes such as vinyl siloxane), polyalkyl aryl siloxanes (eg poly C _1-10 alkyl C _6-20 aryl siloxanes such as polymethylphenyl siloxane, preferably poly C _{1 1- 4} alkyl _{C 6-10} aryl siloxanes), polydiene aryl siloxanes (e.g., polydiene _{C 6-20} aryl siloxanes such as poly diphenyl siloxane), poly alkyl hydrogen siloxane (eg , Poly C _1-10 alkyl siloxane, such as polymethyl hydrogen siloxane), polyorganosiloxane copolymer (e.g., dimethylsiloxane - methylvinylsiloxane copolymer, dimethylsiloxane - methylphenylsiloxane copolymer, dimethylsiloxane - Methylvinylsiloxane-methylphenylsiloxane copolymer, dimethylsiloxane-methylhydrogensiloxane copolymer (dimethicone / methicone copolymer, etc.), modified polyorganosiloxane [modified polyorganosiloxane corresponding to the polyorganosiloxane, eg hydroxyl Modified polyorganosiloxane (eg, terminal silanol polydimethylsiloxane, terminal silanol polymethylphenylsiloxane, terminal hydroxypropyl) Lidimethylsiloxane, polydimethylhydroxyalkylene oxide methylsiloxane, etc.), amino-modified polyorganosiloxane (eg, terminal dimethylaminopolydimethylsiloxane, terminal aminopropylpolydimethylsiloxane), carboxy-modified polyorganosiloxane (eg, terminal carboxypropylpolysiloxane) Dimethylsiloxane, etc.)].

Examples of the organic acid include C5-C30 saturated or unsaturated fatty acids having lauric acid, oleic acid, cetylic acid, stearic acid, ascorbic acid, and palmitic acid.
As the organic amine, oleylamine having C ₁ -C ₃₀ alkyl group, octadecylamine, stearylamine, alkyl amines such as behenyl amine and the aryl amine. It may be a polyethylene glycol functional amine (eg, a Jeffamine material).
In addition to the above, alkyl thiol, aryl thiol, alkyl carboxylic acid, aryl carboxylic acid, alkyl phosphinic acid, aryl phosphinic acid and the like can also be used.
As a treatment method for hydrophobic modification, a method of bringing inorganic particles into contact with the above organic substance and adsorbing the organic substance on the surface of the inorganic particle by a physical / chemical method, or covalent bonding is used.

In the present invention, it has been elucidated that the use of the inorganic particles (d2) suppresses discoloration caused by ultraviolet rays and discoloration caused by heat. The reason for this is not necessarily clear, but it is considered that energy by ultraviolet rays or heat breaks molecular bonds around the nitrogen element and causes coloration.
In the present invention, the inorganic particles (d2) are coated with a resin component comprising a silicone compound (A), a cyclic siloxane compound (B) having a vinyl group, and a hydrosilylation catalyst (C) on a semiconductor element substrate. It has a function of improving. That is, since the inorganic particle (d2) has a hydrocarbon residue derived from an organic substance on the surface thereof, it does not progress hydrogen bonding with the resin component, the adherend surface, and the inorganic particle (d1), so that the coating property is deteriorated over time. Suppress changes. If the amount is too small, the applicability may be deteriorated. If the amount is too large, the adhesive strength and oozing may be adversely affected.

The addition amount of the inorganic particles (d2) is 20 to 80 wt% of the inorganic filler (D). If the addition amount is small and less than 20 wt%, the addition amount of inorganic particles (d1) is relatively increased and the coating property is adversely affected. On the other hand, if the addition amount is more than 80 wt%, the cost of the hydrophobic modification treatment is increased. This is because not only cannot be ignored, but the increase in adhesive strength is small, the viscosity is high, and the applicability deteriorates. A preferable content is 20 to 70 wt%, and further ranges from 20 to 60 wt%.
The silicone resin composition of the present invention containing a predetermined amount of each of the above components has good fluidity, that is, applicability at room temperature (25 ° C.), and is excellent in handling properties. Moreover, as shown in the following examples, the thermal weight loss after 120 minutes at 150 ° C. in the atmosphere is small, and the storage stability at high temperature is excellent.

2. Silicon-containing cured product The silicon-containing cured product of the present invention is a cured product obtained by curing the above-described silicone resin composition.
The curing reaction of the silicone resin composition is a method in which the compounding components of the silicone resin composition of the present invention are separately prepared and mixed immediately before use, and all the compounding components are mixed in advance and heated when performing the curing reaction. There is a method of curing by, and any method may be used.
The heat curing temperature varies depending on the type and amount of the blending component, but is preferably 35 to 350 ° C, more preferably 50 to 250 ° C. Moreover, although hardening time changes also with the kind and quantity of a compounding component, 0.01 to 10 hours are preferable and 0.05 to 6 hours are more preferable.

  By curing reaction of the silicone resin composition of the present invention, it is possible to obtain a cured product having excellent performance such as high adhesiveness, heat resistance, light resistance, and small thermal weight loss.

The silicone compound of component (A) in the present invention is a component (a1) that is a compound having two or more Si-H groups in one molecule, and an unsaturated compound having an alicyclic structure and an ether group (a2 ) Is a prepolymer obtained by hydrosilylation reaction with a component, and by using this as a blending component of the resin composition, low-boiling substances are eliminated, so that a silicon-containing cured product with very little outgas component during the curing reaction It becomes.
Further, in the present invention, since the component (a2) has an alicyclic structure, curing shrinkage is small, and since it has an ether group, it is flexible, so that it becomes a cured product having excellent heat resistance at high temperatures. Furthermore, since the component (a1) according to the present invention is a cyclic siloxane compound, the physical strength (rigidity), crack resistance and the like of the cured product are improved as compared with the case of a chain compound.
It is shown in the following examples, and not only the adhesive strength at room temperature but also the high hot adhesive strength measured when heated to 250 ° C., the cured product was left in an oven at 150 ° C. for 1500 hours. When the transmittance is small, heat resistance is excellent. Further, when the cured product is irradiated with light having a wavelength exceeding 340 nm, the decrease rate of the transmittance at 400 nm is small and the light resistance is excellent.
Further, in the present invention, the inorganic particles (d2) obtained by subjecting the inorganic particles (d1) having a band gap energy of 2.8 eV or more and a refractive index of 1.2 to 1.8 to hydrophobic treatment are specified. The inorganic particles (d2) contain a resin component composed of a silicone compound (A), a cyclic siloxane compound having a vinyl group (B), and a hydrosilylation catalyst (C), with respect to the semiconductor element substrate. It is easy to apply and improves the adhesive strength.

3. Semiconductor Element The silicone resin composition for adhering a semiconductor element of the present invention can be used as an adhesive for blue or white light emitting diode (LED) chips, and can also be used as a sealing resin for semiconductor elements.
At present, in general blue and white LEDs, the substrate is sapphire, and a GaN layer or the like is deposited on the substrate. Generally, since sapphire is an insulator, it cannot conduct vertically, and two electrodes are taken from the GaN layer on the upper surface.
The LED chip needs to be bonded to the lead frame, but the conductive material is not required for the adhesive for the above reason. If it is transparent, the light emitted from the lower surface passes through the transparent adhesive and is reflected by the lead frame surface, and the light can also be output to the outside, thereby increasing the external quantum efficiency. At the same time, if a silicone resin composition is used as an LED sealing resin, the thermal expansion coefficient and the like are the same, so that it can be expected to suppress peeling at the interface between the adhesive and the sealing resin.

  Hereinafter, the present invention will be specifically described using Examples and Comparative Examples, but the present invention is not limited thereto. The raw materials used are as follows.

The silicone compound is obtained by hydrosilylating a cyclic siloxane compound (a1) and an alicyclic unsaturated compound (a2) having a vinyloxy group or an allyloxy group in the manner described in Patent Document 5 (Japanese Patent Laid-Open No. 2009-280747). Things were manufactured.
Silicone compound (A): Hydrosilyl group concentration of 5.0 mmol / g, weight average molecular weight of 150,000, number of Si—H groups per molecule obtained from weight average molecular weight and Si—H group content Was 750.
Cyclic siloxane compound (B) having a vinyl group: 2,4,6,8-tetramethyl-2,4,6,8-tetravinylcyclotetrasiloxane was used.
Hydrosilylation catalyst (C): A platinum-divinyltetramethyldisiloxane complex was used. The silicone compound (A) contains 0.003% of the hydrosilylation catalyst (C).

Inorganic filler (d1) A: Commercially available silicon dioxide powder (manufactured by Tokuyama Corporation, trade name: Leolo Seal). A white powder having a band gap energy of 2.8 eV or more and an average particle diameter of 0.05 μm was used.
Inorganic filler (d1) B: Commercially available aluminum oxide powder (manufactured by Nippon Aerosil Co., Ltd., trade name: AEROXIDE). A white powder having a band gap energy of 2.8 eV or more and an average particle size of 0.03 μm was used.
Inorganic filler (d1) C: Commercially available titanium oxide powder (manufactured by Nippon Aerosil Co., Ltd., trade name: AEROXIDE). A white powder having a band gap energy of 2.8 eV or more and an average particle size of 0.08 μm was used.

Inorganic filler (d2) D: Hydrophobized treated product of commercially available silicon dioxide powder (using dimethyldiethoxysilane as a treating agent). A white powder having a band gap energy of 2.8 eV or more and an average particle diameter of 0.05 μm was used.
Inorganic filler (d2) E: Hydrophobized product of commercially available aluminum oxide powder (dimethyldiethoxysilane is used as a treating agent). A white powder having a band gap energy of 2.8 eV or more and an average particle size of 0.03 μm was used.
Inorganic filler (d2) F: Hydrophobized treated product of commercially available titanium oxide powder (dimethyldimethylsilane is used as a treating agent). A white powder having a band gap energy of 2.8 eV or more and an average particle size of 0.08 μm was used.

Moreover, the evaluation item and evaluation method of a silicone resin composition and its hardened | cured material are as follows.
<Adhesive strength>
The silicone resin composition was dropped onto a stainless steel substrate, a 1.5 mm square silicon chip was placed, and allowed to cure in an oven at 150 ° C. for 120 minutes. After cooling to room temperature, force was applied to the silicon chip from the horizontal direction with respect to the alumina substrate, and the force when the silicon chip was peeled was measured as adhesive strength. If the adhesive strength was 35N or more, it was determined to be acceptable.
<Hot strength>
The silicone resin composition was dropped onto a stainless steel substrate, a 1.5 mm square silicon chip was placed on the stainless steel substrate, and left in an oven at 150 ° C. for 120 minutes to be cured. After cooling to room temperature, the Cu substrate is allowed to stand for 20 seconds on a hot plate heated to 250 ° C., and the silicon chip is pressed from the horizontal direction with respect to the stainless steel substrate while being heated. The force at the time of peeling was measured as the hot strength. If the hot strength was 5N or more, it was considered acceptable.

<Initial transmittance>
The transmittance of 400 nm of the cured product having a thickness of 1 mm was measured using a spectrophotometer. At that time, the initial transmittance was 90% or more: ◎, 80% or more: ◯, 60% or more: Δ, 60% or less: x.
<Heat resistance>
The cured product having a thickness of 1 mm was left in an oven at 150 ° C. for 1500 hours, and the transmittance at 400 nm was measured using a spectrophotometer. At that time, when the rate of decrease in transmittance from the initial stage was less than 5%: ◎, less than 10%: ◯, less than 10-20%: Δ, 20% or more: x.
<Light resistance>
The cured product having a thickness of 1 mm was equipped with a high-pressure mercury lamp fitted with a filter that cuts 340 nm or less, irradiated with 100 mW / cm ² for 24 hours, and the transmittance at 400 nm was measured using a spectrophotometer. At that time, when the rate of decrease from the initial stage was less than 5%: ◎, less than 10%: ◯, less than 10-40%: Δ, 40% or more: x.

<Applicability>
The resin composition filled in the syringe was discharged continuously at 25 points from a needle having an inner diameter of 0.2 mm attached to the syringe discharge port. At that time, the one that is conical or hemispherical is “○”, pulls the thread and touches the adjacent point, extends linearly to the adjacent point, and the conical corner becomes higher When there were 3 or more points that were 2 mm or more, it was determined as “x”.
<Leaching>
The silicone resin composition was dropped onto an alumina substrate, a 1.5 mm square silicon chip was placed on the alumina substrate, and allowed to cure in an oven at 150 ° C. for 120 minutes. After cooling to room temperature, the silicone resin composition of the alumina substrate was observed with a stereomicroscope to confirm whether leaching was observed. When exudation was not recognized: ○, when exudation was observed: x.
<Comprehensive evaluation>
About the obtained sample, adhesive strength, hot strength, initial transmittance, after light resistance test, after heat resistance test, as a result of examining applicability and seepage, adhesive strength is 35 N or more, hot strength is 5 N or more , After initial light transmittance, light resistance test, after heat resistance test, "◎", applicability is "○", exudation is "○", overall evaluation is "○", one of which When there was a characteristic that did not satisfy any one, “x” was assigned.

(Examples 1-8)
Samples of the silicone resin composition of the present invention were prepared by blending the respective raw materials according to the weight ratios in Table 1 and kneading with a three-roll kneader. Using a sample of this silicone resin composition, a cured product was prepared as described above, and the performance was evaluated. The obtained results are also shown in Table 1.
In addition, Example 1 uses the silicone compound (A), the cyclic siloxane compound (B), and the hydrosilylation catalyst (C) produced in the manner described in Patent Document 4 (Japanese Unexamined Patent Application Publication No. 2009-280747). (A) 10 parts by weight of the cyclic siloxane compound, 4.7 parts by weight of the inorganic filler (d1) A, and 7 parts by weight of the hydrophobized inorganic filler (d2) D were blended with 100 parts by weight.
Further, in Example 2, the hydrophobized inorganic filler (d2) D was increased within the scope of the present invention to 9.4 parts by weight, and the inorganic filler (d1) A was reduced to 2.3 parts by weight. A sample of the silicone resin composition of the present invention was produced in the same manner as in Example 1. In Example 3, the inorganic filler (d2) D subjected to the hydrophobization treatment was reduced within the scope of the present invention to 2.3 parts by weight, and the inorganic filler (d1) A was increased to 9.4 parts by weight. In the same manner as in Example 1, a sample of the silicone resin composition of the present invention was produced.
Further, in Example 4, the silicone resin composition of the present invention was the same as in Example 1 except that both the inorganic filler (d2) D and the inorganic filler (d1) A that were hydrophobized were reduced within the scope of the present invention. A sample of the object was made. Example 5 is a sample of the silicone resin composition of the present invention in the same manner as in Example 1 except that both the inorganic filler (d2) D and the inorganic filler (d1) A subjected to hydrophobic treatment were increased within the scope of the present invention. Was made.
In Examples 6-7, instead of the hydrophobic treated inorganic filler (d2) D, the hydrophobic treated inorganic filler (d2) E or the hydrophobic treated inorganic filler (d2) F was used. A silicone resin composition of the present invention was produced in the same manner as in Example 1 using the inorganic filler (d1) B or the inorganic filler (d1) C instead of the filler (d1) A. Furthermore, Example 8 produced the silicone resin composition of this invention like Example 1 using the inorganic filler (d1) C instead of the inorganic filler (d1) A.

(Comparative Examples 1-5)
In contrast to the resin component consisting of the same silicone compound (A), cyclic siloxane compound, and hydrosilylation catalyst as used in Example 1, Comparative Example 1 excluded the hydrophobic filler inorganic filler (d2) D from the scope of the present invention. A sample of a comparative silicone resin composition was prepared in the same manner as in Example 1 except that the content was increased to 9.9 parts by weight and the inorganic filler (d1) A was reduced to 1.8 parts by weight. In Comparative Example 2, the inorganic filler (d2) D subjected to the hydrophobization treatment was reduced to be out of the scope of the present invention, 1.8 parts by weight, and the inorganic filler (d1) A was increased to 9.9 parts by weight. A sample of a comparative silicone resin composition was prepared in the same manner as in Example 1.
Comparative Example 3 is a comparative silicone as in Example 1, except that both the hydrophobic treated inorganic filler (d2) D and inorganic filler (d1) A are reduced outside the scope of the present invention. A sample of the resin composition was prepared. In Comparative Example 4, the inorganic filler (d2) D and the inorganic filler (d1) A that were hydrophobized were both increased outside the scope of the present invention, and Comparative Example 5 was hydrophobized. A sample of a comparative silicone resin composition was prepared without blending the treated inorganic filler (d2) D and inorganic filler (d1) A.
And the cured | curing material was produced in the said way using the sample of these silicone resin compositions, and performance was evaluated. The obtained results are also shown in Table 1. Table 3 shows the relationship between the content ratios of the inorganic filler and the silane coupling agent for reference.

(Comparative Examples 6 to 10)
Instead of the silicone resin composition of Example 1, Comparative Example 6 used T-3925 manufactured by Sumitomo Metal Mining as a general-purpose epoxy resin adhesive. This general-purpose epoxy resin adhesive contains hydrophobic filler-treated inorganic filler (d2) D and inorganic filler (d1) A corresponding to the present invention, but does not contain silicone resin.
In Comparative Example 7, a general-purpose product (KER-3000M2) manufactured by Shin-Etsu Chemical Co., Ltd. was used as a general-purpose silicone resin adhesive. In this general-purpose silicone resin adhesive, an inorganic filler and a silane coupling agent are not added to 100 parts by weight of the resin component. Further, in Comparative Example 8, a sample in which the inorganic filler (d2) D and the inorganic filler (d1) A subjected to the hydrophobic treatment were added to the general-purpose silicone resin adhesive in the same manner as in Example 1. These general-purpose silicone resin adhesives have a structure different from that of the silicone compound (A) of the present invention. Evaluation was performed under the same evaluation conditions as in the Examples, and the obtained evaluation results are shown in Table 2.
Further, Comparative Example 9 was not used for the inorganic filler (d2) D subjected to the hydrophobic treatment with respect to Example 1, and 7 parts by weight of the inorganic filler (d1) B was blended. Comparative Example 10 was a hydrophobic treatment. The inorganic filler (d2) D was not used and 11.7 parts by weight of the inorganic filler (d1) C was blended to prepare a comparative silicone resin composition sample.

"Evaluation"
From Table 1 showing the above results, the examples use the silicone resin composition of the present invention, a specific amount of an inorganic filler is blended with the silicone resin component, and some of the particles are hydrophobized. Therefore, all the performance evaluations are excellent and the comprehensive evaluation is acceptable.
On the other hand, as can be seen from Table 2, in the comparative example, the silicone resin composition of the present invention is different from the amount of inorganic filler and hydrophobized inorganic particles, or the silicone resin component according to the present invention is used. As a result, one of the performance evaluations deteriorates and the overall evaluation fails.

  That is, in Comparative Example 1, as shown in Table 2, since the inorganic particles subjected to the hydrophobization treatment were increased outside the scope of the present invention, leaching occurred. Since the comparative example 2 reduced the inorganic particle hydrophobized outside the range of this invention, the applicability | paintability does not satisfy | fill a request | requirement. In Comparative Example 3, the inorganic filler and the inorganic particles subjected to the hydrophobization treatment were both reduced outside the scope of the present invention, so that the applicability did not satisfy the requirements, and oozing occurred. In Comparative Example 4, both the inorganic filler and the hydrophobized inorganic particles were increased to make them outside the scope of the present invention, so that the applicability did not satisfy the requirements. Since Comparative Example 5 did not contain an inorganic filler and a silane coupling agent, the coatability did not satisfy the requirements, and leaching occurred.

Since the comparative example 6 used the general purpose epoxy resin adhesive with bad light resistance, without using the silicone resin component which concerns on this invention, the performance after a light resistance test and a heat resistance test is falling. In Comparative Example 7, since the general-purpose silicone resin adhesive was used without using the silicone resin component according to the present invention, the adhesive strength characteristics did not satisfy the requirements. Although the comparative example 8 mix | blended the inorganic particle | grain and the inorganic particle hydrophobized in the general purpose silicone resin adhesive, the adhesive strength characteristic does not satisfy | fill a request | requirement.
In Comparative Examples 9 and 10, the inorganic filler was blended with the silicone resin component according to the present invention, but the hydrophobic particles were not blended, so the coating properties did not meet the requirements.

  The silicone resin composition for adhering semiconductor elements of the present invention can be used as an adhesive for blue or white light emitting diode (LED) chips, or as a sealing resin. Since the adhesive is transparent, light emitted on the lower surface of the substrate is transmitted through the transparent adhesive and reflected by the lead frame surface, and the light can also be output to the outside, thereby increasing the external quantum efficiency. When used as a sealing resin for LEDs, the thermal expansion coefficient and the like are the same, so peeling at the interface between the adhesive and the sealing resin is small.

Claims (6)

Silicone compound (A) obtained by hydrosilylating cyclic siloxane compound (a1) and alicyclic unsaturated compound (a2) having vinyloxy group or allyloxy group, cyclic siloxane compound (B) having vinyl group, hydrosilylation catalyst A silicone resin composition for adhering semiconductor elements, comprising a resin component comprising (C) and an inorganic filler (D) which is a mixture of inorganic particles (d1) and inorganic particles (d2) ,
Inorganic particles (d1) and inorganic particles (d2) is, silicon fluoride, magnesium oxide, aluminum oxide, silicon dioxide, zirconium oxide or one or more which are identical or different species selected from titanium oxide, inorganic particles ( d1) is not subjected to hydrophobic treatment, whereas inorganic particles (d2) are subjected to hydrophobic treatment, and the content of the inorganic filler (D) is (A), (B) and (C). ) Silicone for bonding semiconductor elements, characterized in that the total amount of the components is 0.1 to 40 parts by weight, and the proportion of the inorganic particles (d2) is 20 to 80 wt% of the inorganic filler (D). Resin composition.   2. The silicone resin composition for adhering a semiconductor element according to claim 1, wherein the silicone compound (A) has a hydrosilyl group concentration of 1 to 10 mmol / g.   The silicone resin composition for bonding a semiconductor element according to claim 1, wherein the hydrosilylation catalyst (C) is a platinum-based catalyst.   2. The silicone resin for bonding a semiconductor element according to claim 1, wherein the inorganic filler (D) is an inorganic particle having a band gap energy of 2.8 eV or more and a refractive index of 1.2 to 1.8. Composition.   The inorganic particles (d2) are subjected to hydrophobic modification treatment with one or more organic substances selected from alcohols having 1 to 20 carbon atoms, organic silyl compounds, organic acids, or organic amines. The silicone resin composition for semiconductor element adhesion as described.   A silicon-containing cured product obtained by heat-curing the silicone resin composition according to claim 1.