JP5605394B2 - Epoxy resin composition for semiconductor encapsulation and semiconductor device - Google Patents

Description

  The present invention relates to an epoxy resin composition for semiconductor encapsulation and a semiconductor device using the same, and in particular, an epoxy resin composition for semiconductor encapsulation having characteristics excellent in fluidity, releasability, and continuous moldability, and The present invention relates to a semiconductor device using the same and having excellent solder reflow resistance.

  In recent years, as electronic devices are required to be advanced, lightened, thinned, and downsized, semiconductor devices have been highly integrated and surface-mounted. As a result, the demand for epoxy resin compositions for semiconductor encapsulation is becoming increasingly severe. In particular, when the semiconductor device is made thinner, stress is generated due to insufficient release between the mold and the cured product of the epoxy resin composition. This stress may cause cracks in the semiconductor element itself in the semiconductor device, or may decrease the adhesion at the interface between the cured product and the semiconductor element. For this reason, the mold release property which can be easily released from the mold is required for the molded body (cured product) obtained from the epoxy resin composition. Further, from the viewpoint of productivity, it has been demanded that a molded body can be continuously formed (continuous moldability).

  In addition, while the influence on the environment is regarded as a problem, there is a shift from leaded solder to lead-free solder. Lead-free solder has a higher temperature at the time of solder processing than leaded solder, and very high stress may be generated due to evaporation of moisture contained in the semiconductor device. Thus, the solder reflow resistance of the molded body has become a bigger problem than before.

  Various proposals for improving the solder reflow resistance have been made. For example, an epoxy resin composition containing a high-concentration inorganic filler and a biphenyl type epoxy resin, which is a low viscosity type epoxy resin, has been proposed (see Patent Documents 1 and 2). Since this epoxy resin composition contains many inorganic fillers, fluidity | liquidity falls. Thus, the solder reflow resistance of the molded product and the fluidity of the epoxy resin composition for semiconductor encapsulation are in a trade-off relationship.

  Therefore, an epoxy resin composition for semiconductor encapsulation having excellent fluidity, releasability, continuous moldability, etc., and also excellent cured properties such as solder reflow resistance, and a semiconductor element are encapsulated with the composition. There is a need for a semiconductor device.

JP-A-5-131486 (pages 1-9) JP-A-8-253555 (pages 2-9)

  The present invention has been made in view of the above circumstances, and its purpose is excellent in fluidity, releasability, continuous formability, etc., and also in semiconductor encapsulation excellent in cured product properties such as solder reflow resistance. An epoxy resin composition for use, and a semiconductor device in which a semiconductor element is sealed with the composition.

The present invention
[1] (A) epoxy resin, (B) phenol resin, (C) curing accelerator, (D) inorganic filler, (E2) glycerin trifatty acid ester , (F) silane coupling agent, and (G) aroma A compound in which a hydroxyl group is bonded to each of two or more adjacent carbon atoms constituting a ring,
At least one of the epoxy resin (A) and the phenol resin (B) is represented by the following general formula (1)

(In the general formula (1), R is a group selected from a hydrogen atom or an alkyl group having 1 to 4 carbon atoms, and a plurality of R may be the same or different from each other. , Glycidyl ether group or hydroxyl group, n is an average value and is a positive number of 1 to 3.)
Including a resin represented by
The total epoxy resin composition contains 0.01% by weight or more and 1% by weight or less of the glycerin trifatty acid ester (E2), and 0.01% by weight or more and 1% by weight or less of the compound (G). An epoxy resin composition for semiconductor encapsulation.

  [2] The compound (G) is represented by the following general formula (2):

(In the general formula (2), one of R ₁ and R ₅ is a hydroxyl group, and when one is a hydroxyl group, the other is a hydrogen atom, a hydroxyl group, or a substituent other than a hydroxyl group. R ₂ , R ₃ , R ₄ may be each independently a hydrogen atom, a hydroxyl group, or a substituent other than a hydroxyl group, or R ₂ and R ₃ , or R ₃ and R ₄ may combine to form an aromatic ring. The epoxy resin composition for semiconductor encapsulation according to [1], which is represented by:

[3] The epoxy resin composition for semiconductor encapsulation according to [1] or [2], wherein the dropping point of the glycerin trifatty acid ester (E2) is 70 ° C. or higher and 120 ° C. or lower.

[ 4 ] The glycerin trifatty acid ester (E2) has an average particle size of 20 μm or more and 70 μm or less, and the content ratio of particles having a particle size of 106 μm or more in the total glycerin trifatty acid ester (E2) is 0.1% by weight or less. The epoxy resin composition for semiconductor encapsulation according to any one of [1] to [3].

[ 5 ] The epoxy resin composition for semiconductor encapsulation according to any one of [1] to [4], wherein the acid value of the glycerin trifatty acid ester (E2) is 10 mgKOH / g or more and 50 mgKOH / g or less.
[6] The semiconductor sealing epoxy according to any one of [1] to [5], wherein the glycerin trifatty acid ester (E2) is a triester compound of glycerin and a saturated fatty acid having 24 to 36 carbon atoms. Resin composition.

[7] (A) Epoxy resin,
(B) phenolic resin,
(C) a curing accelerator,
(D) inorganic filler,
(E3) oxidized paraffin wax,
(F) a silane coupling agent, and
(G) A compound in which a hydroxyl group is bonded to each of two or more adjacent carbon atoms constituting an aromatic ring.
Including
At least one of the epoxy resin (A) and the phenol resin (B) is represented by the following general formula (1)

(In the general formula (1), R is a group selected from a hydrogen atom or an alkyl group having 1 to 4 carbon atoms, and a plurality of R may be the same or different from each other. , Glycidyl ether group or hydroxyl group, n is an average value and is a positive number of 1 to 3.)
Including a resin represented by
  The total epoxy resin composition contains 0.01% by weight to 1% by weight of the oxidized paraffin wax (E3) and 0.01% by weight to 1% by weight of the compound (G). An epoxy resin composition for semiconductor encapsulation.

[8] The compound (G) is represented by the following general formula (2):

(In the above general formula (2), R ₁ , R ₅ Is a hydroxyl group, and when one is a hydroxyl group, the other is a hydrogen atom, a hydroxyl group, or a substituent other than a hydroxyl group. R ₂ , R ₃ , R ₄ Each independently may be a hydrogen atom, a hydroxyl group, or a substituent other than a hydroxyl group, and R ₂ And R ₃ Or R ₃ And R ₄ May combine to form an aromatic ring. ] The epoxy resin composition for semiconductor encapsulation as described in [7].

[9] The epoxy resin composition for semiconductor encapsulation according to [7] or [8], wherein the oxidized paraffin wax (E3) has a softening point of 70 ° C. or higher and 120 ° C. or lower.

[10] The average particle diameter of the oxidized paraffin wax (E3) is 20 μm or more and 70 μm or less, and the content ratio of particles having a particle diameter of 106 μm or more in the total oxidized paraffin wax (E3) is 0.1 wt% or less. 7] thru | or the epoxy resin composition for semiconductor sealing in any one of [9].

[11] The epoxy resin composition for semiconductor encapsulation according to any one of [7] to [10], wherein the acid value of the oxidized paraffin wax (E3) is 10 mgKOH / g or more and 50 mgKOH / g or less.

[12] A semiconductor device comprising a semiconductor element sealed using the epoxy resin composition for semiconductor sealing according to any one of [1] to [11].

  According to the present invention, an epoxy resin composition for semiconductor encapsulation having excellent fluidity, releasability, continuous moldability, and the like, and further excellent cured product properties such as solder reflow resistance and moisture absorption, and the resin composition Thus, a semiconductor device in which a semiconductor element is sealed can be provided.

The epoxy resin composition for semiconductor encapsulation of the present invention contains the following components (A) to (G).
(A) Epoxy resin (B) Phenol resin (C) Curing accelerator (D) Inorganic filler (E) Release agent (F) Silane coupling agent (G) Two or more adjacent carbons constituting an aromatic ring Compounds with hydroxyl groups attached to each atom

Furthermore, in the epoxy resin composition for semiconductor encapsulation of the present invention, the epoxy resin (A) and the phenol resin (B) satisfy any one of the requirements (i) to (iii) in the following general formula (1). Fulfill.
(I) The epoxy resin (A) includes an epoxy resin in which X is represented by a glycidyl ether group in the following general formula (1).
(Ii) The phenol resin (B) includes a phenol resin in which X is a hydroxyl group in the following general formula (1).
(Iii) Satisfy any of the requirements (i) and (ii) above.

(In the general formula (1), R is a group selected from a hydrogen atom or an alkyl group having 1 to 4 carbon atoms, and a plurality of R may be the same or different from each other. , Glycidyl ether group or hydroxyl group, n is an average value and is a positive number of 1 to 3.)

  Furthermore, the mold release agent (E) is a compound selected from the group consisting of oxidized polyethylene wax (E1), glycerin trifatty acid ester (E2) and oxidized paraffin wax (E3). Further, the total epoxy resin composition contains the release agent (E) in an amount of 0.01% by weight to 1% by weight and the compound (G) in an amount of 0.01% by weight to 1% by weight.

The epoxy resin composition for semiconductor encapsulation of the present invention is excellent in fluidity, releasability and continuous moldability when encapsulating a semiconductor element, etc. due to the composition as described above, and further has solder reflow resistance. Excellent cured product properties such as low hygroscopicity, low stress, and adhesion to metal-based members.
Hereinafter, the epoxy resin composition for semiconductor encapsulation of the present invention (hereinafter also simply referred to as “epoxy resin composition”) will be described in detail.

<Epoxy resin (A)>
The epoxy resin (A) used in the present invention is represented by the following general formula (a) wherein X is a glycidyl ether group in the general formula (1).

(In the general formula (a), R is a group selected from a hydrogen atom or an alkyl group having 1 to 4 carbon atoms, and a plurality of R may be the same or different from each other. (The average value is a positive number from 1 to 3.)
It is preferable that the epoxy resin represented by these is included. In the general formula (a), it is more preferable that a plurality of Rs are all hydrogen atoms.

  The epoxy resin represented by the general formula (a) includes many hydrophobic structures in the resin skeleton. Therefore, the hardened | cured material obtained from the epoxy resin composition containing this epoxy resin has a low moisture absorption, and can suppress generation | occurrence | production of the very high stress by the vaporization of the water | moisture content at the time of solder reflow. Furthermore, since the crosslink density of the cured product is low and the elastic modulus is low in a high temperature range above the glass transition temperature, the thermal stress generated during the soldering process is reduced, resulting in excellent solder reflow resistance.

In this invention, it can use together with another epoxy resin in the range which does not impair the effect by using the epoxy resin of the said General formula (1). Examples of other epoxy resins include phenol novolac type epoxy resins, cresol novolac type epoxy resins, biphenyl type epoxy resins, bisphenol type epoxy resins, stilbene type epoxy resins, triphenolmethane type epoxy resins, and phenol aralkyls (including phenylene skeletons). Type epoxy resin, naphthol type epoxy resin, alkyl-modified triphenolmethane type epoxy resin, triazine nucleus-containing epoxy resin, dicyclopentadiene-modified phenol type epoxy resin, and the like. These other epoxy resins may be used alone or in combination.
When not using the epoxy resin of the said general formula (a) as an epoxy resin (A), said other epoxy resin can be used. In addition, when not using the epoxy resin of the said general formula (a), it is preferable to use the phenol resin represented by the general formula (b) mentioned later as a phenol resin (B).

<Phenolic resin (B)>
The phenol resin (B) used in the present invention is represented by the following general formula (b) wherein X is a hydroxyl group in the general formula (1).

(In the general formula (b), R is a group selected from a hydrogen atom or an alkyl group having 1 to 4 carbon atoms, and a plurality of R may be the same or different from each other. The average value is a positive number of 1 to 3). In the general formula (b), it is more preferable that a plurality of Rs are all hydrogen atoms.

  The phenol resin represented by the general formula (b) contains a lot of hydrophobic structures in the resin skeleton. Therefore, the hardened | cured material obtained from the epoxy resin composition containing this phenol resin has a low moisture absorption, and can suppress generation | occurrence | production of the very high stress by the vaporization of the water | moisture content at the time of solder reflow. Furthermore, since the crosslink density of the cured product is low and the elastic modulus is low in a high temperature range above the glass transition temperature, the thermal stress generated during the soldering process is reduced, resulting in excellent solder reflow resistance.

  In this invention, it can use together with another phenol resin in the range which does not impair the effect by using the phenol resin of the said general formula (b). Examples of other phenol resins include phenol novolac resins, cresol novolac resins, triphenol methane resins, terpene modified phenol resins, dicyclopentadiene modified phenol resins, phenol aralkyl resins (including phenylene skeletons), naphthol aralkyl resins, and the like. Can do. These other phenol resins may be used alone or in combination.

  When not using the phenol resin of the said general formula (b) as a phenol resin (B), said other phenol resin can be used. In addition, when not using the phenol resin of the said general formula (b), it is preferable to use the epoxy resin represented by general formula (a) as said epoxy resin (A).

  The equivalent ratio of epoxy groups of all epoxy resins and phenolic hydroxyl groups of all phenol resins used in the present invention is preferably 0.5 or more and 2 or less, particularly preferably 0.7 or more and 1.5 or less. . If it exists in the said range, while the epoxy resin composition is excellent in sclerosis | hardenability, the hardened | cured material obtained from this composition is excellent in moisture resistance.

<Curing accelerator (C)>
As a hardening accelerator (C) used by this invention, what can become a catalyst of the crosslinking reaction of an epoxy resin and a phenol resin can be used. Examples of the curing accelerator (C) include organic compounds such as tributylamine, amine compounds such as 1,8-diazabicyclo (5,4,0) undecene-7, triphenylphosphine, tetraphenylphosphonium / tetraphenylborate salts, and the like. Examples thereof include, but are not limited to, imidazole compounds such as 2-methylimidazole. These curing accelerators may be used alone or in combination.

<Inorganic filler (D)>
Examples of the inorganic filler (D) used in the present invention include fused silica, crystalline silica, alumina, silicon nitride, and aluminum nitride. When the amount of the inorganic filler is particularly large, it is preferable to use fused silica.

  Fused silica can be used in either crushed or spherical shape, but in order to increase the blending amount of fused silica and to suppress the increase in melt viscosity of the epoxy resin composition, the spherical one is mainly used. Is preferred. In order to further increase the blending amount of the spherical silica, it is desirable to adjust so that the particle size distribution of the spherical silica becomes wider.

<Release agent (E)>
Examples of the release agent (E) used in the present invention include oxidized polyethylene wax (E1), glycerin trifatty acid ester (E2), and oxidized paraffin wax (E3). These release agents may be used alone or in combination.
Hereinafter, these release agents will be described in order.

(Oxidized polyethylene wax (E1))
Since the oxidized polyethylene wax (E1) generally has a polar group composed of carboxylic acid and the like and a nonpolar group composed of a long carbon chain, the polar group is oriented toward the resin cured product during molding, In addition, the nonpolar group acts as a release agent by being oriented on the mold side.

  The content of the oxidized polyethylene wax (E1) in the epoxy resin composition is 0.01% by weight or more and 1% by weight or less, preferably 0.03% by weight or more and 0.5% by weight or less. It is excellent in the mold release property of the hardened | cured material from a metal mold | die within the said range. Furthermore, since the adhesiveness with the lead frame member is excellent, peeling between the lead frame member and the cured product can be suppressed during the soldering process. In addition, it is possible to suppress deterioration of the mold and the appearance of the cured product during molding.

  Examples of the oxidized polyethylene wax (E1) include an oxide of polyethylene wax produced by a low pressure polymerization method, an oxide of polyethylene wax produced by a high pressure polymerization method, and an oxide of a high density polyethylene polymer. Among these, an oxide of a high density polyethylene polymer is more preferable. These oxidized polyethylene waxes may be used alone or in combination.

  The following are (1-1) dropping point, (1-2) acid value, (1-3) number average molecular weight, (1-4) density, (1-5) average particle diameter of oxidized polyethylene wax (E1). (1-6) The content ratio of particles having a particle size of 106 μm or more will be described in order.

(1-1) Dropping point The dropping point of the oxidized polyethylene wax (E1) is 100 ° C. or higher and 140 ° C. or lower, preferably 110 ° C. or higher and 130 ° C. The dropping point can be measured by a method based on ASTM D127. Specifically, using a metal nipple, it is measured as the temperature at which molten wax first drops from the metal nipple. In the following examples, it can be measured by the same method.

  When the dropping point is within the above range, the oxidized polyethylene wax (E1) is excellent in thermal stability, and the oxidized polyethylene wax (E1) is hardly seized at the time of molding. Therefore, it is excellent in the mold release property of the hardened | cured material from a metal mold | die, and is excellent also in continuous moldability. Furthermore, when it is within the above range, the oxidized polyethylene wax (E1) is sufficiently melted when the epoxy resin composition is cured. Thereby, the oxidized polyethylene wax is dispersed substantially uniformly in the cured product. Therefore, segregation of the oxidized polyethylene wax (E1) on the surface of the cured product is suppressed, and deterioration of the mold stain and the appearance of the cured product can be reduced.

(1-2) Acid value The acid value of the oxidized polyethylene wax (E1) is from 10 mgKOH / g to 50 mgKOH / g, preferably from 15 mgKOH / g to 40 mgKOH / g. The acid value affects the compatibility in the cured product. The acid value can be measured by a method based on JIS K 3504. Specifically, it is measured as the number of milligrams of potassium hydroxide required to neutralize free fatty acids contained in 1 g of waxes. In the following examples, it can be measured by the same method.

  When the acid value is within the above range, the oxidized polyethylene wax (E1) is in a compatible state with the epoxy resin matrix in the cured product. Thereby, the oxidized polyethylene wax (E1) and the epoxy resin matrix do not cause phase separation. Therefore, segregation of the oxidized polyethylene wax (E1) on the surface of the cured product is suppressed, and deterioration of the mold stain and the appearance of the cured product can be reduced.

  Furthermore, since the oxidized polyethylene wax (E1) is present on the surface of the cured product, the releasability of the cured product from the mold is excellent. On the other hand, if the compatibility between the oxidized polyethylene wax (E1) and the epoxy resin matrix is too high, the oxidized polyethylene wax (E1) cannot ooze out on the surface of the cured product, and sufficient releasability cannot be ensured. There is a case.

(1-3) Number average molecular weight The number average molecular weight of the oxidized polyethylene wax (E1) is 500 or more and 5000 or less, preferably 1000 or more and 4000 or less. The number average molecular weight can be calculated by polystyrene conversion using a GPC apparatus such as HLC-8120 manufactured by Tosoh Corporation. In the following examples, it can be measured by the same method.

  When the number average molecular weight is within the above range, the oxidized polyethylene wax (E1) and the epoxy resin matrix are in a preferable affinity state. Therefore, the cured product is excellent in releasability from the mold. On the other hand, if the affinity between the oxidized polyethylene wax (E1) and the epoxy resin matrix is high, sufficient releasability may not be obtained. On the other hand, if the affinity is low, phase separation may occur, and the mold may become dirty or the appearance of the cured resin may be deteriorated.

(1-4) Density The density of the oxidized polyethylene wax (E1) is 0.94 g / cm ³ or more and 1.03 g / cm ³ or less, preferably 0.97 g / cm ³ or more, 0.99 g / cm ^3. It is as follows. The density can be calculated by density measurement at 20 ° C. by a floating method based on ASTM D1505. In the following examples, it can be measured by the same method.

  When the density is within the above range, the oxidized polyethylene wax (E1) is excellent in thermal stability, and the oxidized polyethylene wax (E1) is hardly seized at the time of molding. Therefore, it is excellent in the mold release property of the hardened | cured material from a metal mold | die, and is excellent also in continuous moldability. Furthermore, when the epoxy resin composition is cured within the above range, the oxidized polyethylene wax (E1) is sufficiently melted. Thereby, the oxidized polyethylene wax (E1) is dispersed substantially uniformly in the cured product. Therefore, segregation of the oxidized polyethylene wax (E1) on the surface of the cured product is suppressed, and deterioration of the mold stain and the appearance of the cured product can be reduced.

(1-5) Average particle diameter The average particle diameter is 20 μm or more and 70 μm or less, preferably 30 μm or more and 60 μm or less. The average particle diameter can be measured by using a laser diffraction particle size distribution measuring device such as SALD-7000 manufactured by Shimadzu Corporation as a solvent and water, and a weight-based 50% particle diameter as an average particle diameter. it can. In the following examples, it can be measured by the same method.

  When the average particle size is within the above range, the oxidized polyethylene wax (E1) is in a compatible state with the epoxy resin matrix in the cured product. Thereby, the oxidized polyethylene wax (E1) is present on the surface of the cured product, and the release property of the cured product from the mold is excellent. On the other hand, if the compatibility with the epoxy resin matrix is too high, the cured product surface cannot be oozed out and sufficient releasability cannot be ensured.

  Further, since the oxidized polyethylene wax (E1) and the epoxy resin matrix are in a preferable compatible state, segregation of the oxidized polyethylene wax (E1) on the surface of the cured product is suppressed, and the mold stains and the appearance of the cured product are deteriorated. Can be reduced.

  Furthermore, when it is in the above range, the oxidized polyethylene wax (E1) is sufficiently melted when the epoxy resin composition is cured. Therefore, the epoxy resin composition is excellent in fluidity.

(1-6) Content ratio of particles having a particle size of 106 μm or more The content ratio of particles having a particle size of 106 μm or more in the total oxidized polyethylene wax (E1) is preferably 0.1% by weight or less. This content ratio can be measured using a standard sieve of 106 μm openings according to JIS Z8801. In the following examples, it can be measured by the same method.

  If it is said content ratio, oxidized polyethylene wax (E1) will disperse | distribute substantially uniformly, and the deterioration of the external appearance of a mold | die stain | pollution | contamination and a resin cured material can be suppressed. In addition, when the epoxy resin composition is cured, the oxidized polyethylene wax is sufficiently melted, and thus has excellent fluidity.

  In the present invention, other mold release agents can be used in combination as long as the effect of using the oxidized polyethylene wax (E1) is not impaired. Examples of other release agents that can be used in combination include natural waxes such as carnauba wax and metal salts of higher fatty acids such as zinc stearate.

(Glycerin trifatty acid ester (E2))
Glycerin trifatty acid ester (E2) is a triester obtained from glycerin and saturated fatty acid. When the epoxy resin composition contains glycerin trifatty acid ester (E2), the releasability of the cured product obtained from the composition is very excellent. On the other hand, monoesters and diesters of glycerin and saturated fatty acids are preferred because the moisture resistance of the cured product obtained from the epoxy resin composition is lowered due to the influence of the remaining hydroxyl group, and as a result, the solder reflow resistance is adversely affected. Absent.

  The content of glycerin trifatty acid ester (E2) in the epoxy resin composition is 0.01% by weight or more and 1% by weight or less, preferably 0.03% by weight or more and 0.5% by weight or less. It is excellent in the mold release property of the hardened | cured material from a metal mold | die within the said range. Furthermore, since the adhesiveness with the lead frame member is excellent, peeling between the lead frame member and the cured product can be suppressed during the soldering process. In addition, it is possible to suppress deterioration of the mold and the appearance of the cured resin.

  Examples of the glycerin trifatty acid ester (E2) include glycerin tricaproic acid ester, glycerin tricaprylic acid ester, glycerin tricapric acid ester, glycerin trilauric acid ester, glycerin trimyristic acid ester, glycerin tripalmitic acid ester, glycerin tristearic acid ester. Examples thereof include acid esters, glycerin triaraquinic acid esters, glycerin tribehenic acid esters, glycerin trilignoceric acid esters, glycerin triserotinic acid esters, glycerin trimontanic acid esters, and glycerin trimellitic acid esters. These glycerin trifatty acid esters may be used alone or in combination.

  Among these, glycerin and a glycerin trifatty acid ester of a saturated fatty acid having 24 to 36 carbon atoms are preferable from the viewpoints of releasability and appearance of the molded body. Furthermore, glycerin trimontanic acid ester is more preferable. In the present invention, the carbon number of the saturated fatty acid refers to the sum of the carbon number of the alkyl group and the carboxyl group in the saturated fatty acid.

  The following is the content ratio of (2-1) dropping point, (2-2) acid value, (2-3) average particle diameter, and (2-4) particle diameter of 106 μm or more of glycerin trifatty acid ester (E2). , Will be explained.

(2-1) Dropping point The dropping point of glycerin trifatty acid ester (E2) is preferably 70 ° C. or higher and 120 ° C. or lower, more preferably 80 ° C. or higher and 110 ° C. or lower.

  When the dropping point is within the above range, the glycerin trifatty acid ester (E2) is excellent in thermal stability, and the glycerin trifatty acid ester (E2) is difficult to seize at the time of molding. Therefore, it is excellent in the mold release property of the hardened | cured material from a metal mold | die, and is excellent also in continuous moldability. Further, when the epoxy resin composition is cured within the above range, the glycerin trifatty acid ester (E2) is sufficiently melted. Thereby, glycerol tri fatty acid ester (E2) disperse | distributes substantially uniformly in hardened | cured material. Therefore, segregation of glycerin trifatty acid ester (E2) on the surface of the cured product is suppressed, and deterioration of the appearance of the mold and the cured product can be reduced.

(2-2) Acid Value The acid value of glycerin trifatty acid ester (E2) is preferably 10 mgKOH / g or more and 50 mgKOH / g or less, more preferably 15 mgKOH / g or more and 40 mgKOH / g or less. The acid value affects the compatibility in the cured product.

  When it exists in the said range, glycerol tri fatty-acid ester (E2) will be in a compatible state with an epoxy resin matrix in a hardened | cured material. Thereby, phase separation does not raise | generate a glycerol tri fatty acid ester (E2) and an epoxy resin matrix. Therefore, segregation of glycerin trifatty acid ester (E2) on the surface of the cured product is suppressed, and deterioration of the appearance of the mold and the cured product can be reduced.

  Furthermore, since glycerin trifatty acid ester (E2) is present on the surface of the cured product, the cured product is excellent in releasability from the mold. On the other hand, if the compatibility with the epoxy resin matrix is too high, the glycerin trifatty acid ester (E2) cannot ooze out on the surface of the cured product, and sufficient releasability may not be ensured.

(2-3) Average particle diameter The average particle diameter is preferably 20 μm or more and 70 μm or less, more preferably 30 μm or more and 60 μm or less.

  When it exists in the said range, glycerol tri fatty-acid ester (E2) will be in a compatible state with an epoxy resin matrix in a hardened | cured material. Thereby, glycerol trifatty acid ester (E2) exists in the hardened | cured material surface, and is excellent in the mold release property of the hardened | cured material from a metal mold | die. On the other hand, if the compatibility with the epoxy resin matrix is too high, the cured product surface cannot be oozed out and sufficient releasability cannot be ensured.

  Further, since the glycerin trifatty acid ester (E2) and the epoxy resin matrix are in a preferable compatible state, segregation of the glycerin trifatty acid ester (E2) on the surface of the cured product is suppressed, and the mold dirt and the appearance of the cured product are suppressed. Can be reduced.

Furthermore, when it exists in the said range, when hardening an epoxy resin composition, glycerol tri-fatty acid ester (E2) will fully fuse | melt. Therefore, the epoxy resin composition is excellent in fluidity.
(2-4) Content ratio of particles having a particle size of 106 μm or more The content ratio of particles having a particle size of 106 μm or more in the total glycerin trifatty acid ester is preferably 0.1% by weight or less.

  If it is said content ratio, glycerol tri-fatty acid ester (E2) will disperse | distribute substantially uniformly in an epoxy resin composition, and it can suppress the deterioration of the external appearance of a mold | die stain | pollution | contamination and a resin cured material. In addition, when the epoxy resin composition is cured, the oxidized polyethylene wax is sufficiently melted, and thus has excellent fluidity.

  The glycerin trifatty acid ester used in the present invention is commercially available, and can be used after adjusting the particle size. Other release agents can be used in combination as long as the effects of using the glycerin trifatty acid ester used in the present invention are not impaired. Examples of release agents that can be used in combination include natural waxes such as carnauba wax, and metal salts of higher fatty acids such as zinc stearate.

(Oxidized paraffin wax (E3))
Oxidized paraffin wax (E3) is a general term for oxides obtained by oxidizing paraffin wax by air oxidation or acid addition. By being oxidized, carboxyl groups are introduced into the paraffin wax. The raw material paraffin wax is a product obtained by separating and purifying a vacuum distilled oil, and is a solid wax at room temperature. Usually, the carbon number is 20 or more and 40 or less, and the molecular weight is 300 or more and 550 or less.

  The content of the oxidized paraffin wax (E3) in the epoxy resin composition is 0.01% by weight or more and 1% by weight or less, preferably 0.03% by weight or more and 0.5% by weight or less. When it is within the above range, the cured product obtained from the epoxy resin composition is excellent in releasability from the mold. Furthermore, since the adhesiveness with the lead frame member is excellent, peeling between the lead frame member and the cured product can be suppressed during the soldering process. In addition, it is possible to suppress deterioration of the mold and the appearance of the cured resin.

  Below, (3-1) softening point of oxidized paraffin wax (E3), (3-2) acid value, (3-3) average particle diameter, (3-4) content ratio of particles having a particle diameter of 106 μm or more, Will be explained.

(3-1) Softening point The softening point of the oxidized paraffin wax (E3) is preferably 70 ° C or higher and 120 ° C or lower, more preferably 80 ° C or higher and 110 ° C or lower. The softening point can be measured according to JIS K-2235-5.3.1.

  When the softening point is within the above range, the oxidized paraffin wax (E3) is excellent in thermal stability, and the oxidized paraffin wax (E3) is hardly seized at the time of molding. Therefore, it is excellent in the mold release property of the hardened | cured material from a metal mold | die, and is excellent also in continuous moldability. Furthermore, when it is within the above range, the oxidized paraffin wax (E3) is sufficiently melted when the epoxy resin composition is cured. Thereby, the oxidized paraffin wax (E3) is dispersed substantially uniformly in the cured product. Therefore, segregation of the oxidized paraffin wax (E3) on the surface of the cured product is suppressed, and deterioration of the mold stain and the appearance of the cured product can be reduced.

(3-2) Acid value The acid value is preferably 10 mgKOH / g or more and 50 mgKOH / g or less, more preferably 15 mgKOH / g or more and 40 mgKOH / g or less. The acid value affects the compatibility in the cured product.

  When the acid value is within the above range, the oxidized paraffin wax (E3) is in a preferable compatible state with the epoxy resin matrix in the cured product. Thereby, the oxidized paraffin wax (E3) and the epoxy resin matrix do not cause phase separation. Therefore, segregation of the oxidized paraffin wax (E3) on the surface of the cured product is suppressed, and deterioration of the mold stain and the appearance of the cured product can be reduced.

  Furthermore, since the oxidized paraffin wax (E3) is present on the surface of the cured product, the releasability of the cured product from the mold is excellent. On the other hand, if the compatibility with the epoxy resin matrix is too high, the cured product surface cannot be oozed out and sufficient releasability may not be ensured.

(3-3) Average particle diameter The average particle diameter is preferably 20 μm or more and 70 μm or less, more preferably 30 μm or more and 60 μm or less.

  When the average particle size is within the above range, the oxidized paraffin wax (E3) is in a preferable compatible state with the epoxy resin matrix in the cured product. Thereby, the oxidized paraffin wax (E3) is present on the surface of the cured product, and the releasability of the cured product from the mold is excellent. On the other hand, if the compatibility with the epoxy resin matrix is too high, the cured product surface cannot be oozed out and sufficient releasability cannot be ensured.

  Furthermore, since the oxidized paraffin wax (E3) and the epoxy resin matrix are in a preferable compatible state, segregation of the oxidized paraffin wax (E3) on the surface of the cured product is suppressed, and the mold dirt and the appearance of the cured product are deteriorated. Can be reduced.

  Furthermore, when it is in the above range, the oxidized paraffin wax (E3) is sufficiently melted when the epoxy resin composition is cured. Therefore, the epoxy resin composition is excellent in fluidity.

(3-4) Content ratio of particles having a particle diameter of 106 μm or more The content ratio of particles having a particle diameter of 106 μm or more in the total oxidized paraffin wax (E3) is preferably 0.1% by weight or less.

  If it is said content ratio, oxidized paraffin wax (E3) will disperse | distribute substantially uniformly and it can suppress the deterioration of the external appearance of the mold | die stain | pollution | contamination and resin hardened | cured material by segregation of oxidized paraffin wax (E3). In addition, when the epoxy resin composition is cured, the oxidized paraffin wax (E3) is sufficiently melted, so that the fluidity is excellent.

  The oxidized paraffin wax (E3) used in the present invention is commercially available and can be used after adjusting the particle size. In the present invention, other mold release agents can be used in combination as long as the effect of using the oxidized paraffin wax (E3) is not impaired. Examples of release agents that can be used in combination include natural waxes such as carnauba wax, and metal salts of higher fatty acids such as zinc stearate.

<Silane coupling agent (F)>
The silane coupling agent (F) is not particularly limited, and a silane coupling agent (F) that reacts between an organic component such as an epoxy resin or a phenol resin and an inorganic filler to improve the interfacial strength can be used. Specific examples include epoxy silane, amino silane, ureido silane, mercapto silane, and the like. These silane coupling agents (F) may be used alone or in combination. The silane coupling agent (F) is an essential component capable of remarkably improving the viscosity characteristics and flow characteristics of the epoxy resin composition by a synergistic effect with the compound (G) described later.

  The amount of the silane coupling agent (F) used in the present invention is 0.01% by weight or more and 1% by weight or less, preferably 0.05% by weight or more and 0.8 or less, particularly preferably 0% in the total epoxy resin composition. .1% by weight or more and 0.6% by weight or less. Within the above range, the effect of the compound (G) described later is sufficiently obtained, and the solder reflow resistance in the semiconductor package is improved. Furthermore, the water absorption of the epoxy resin composition is suppressed, and the solder reflow resistance in the semiconductor package is improved.

<Compound (G) in which a hydroxyl group is bonded to each of two or more adjacent carbon atoms constituting an aromatic ring>
A compound (G) in which a hydroxyl group is bonded to each of two or more adjacent carbon atoms constituting an aromatic ring (hereinafter referred to as compound (G)) has the following general formula (2)

(In the general formula (2), one of R ₁ and R ₅ is a hydroxyl group, and when one is a hydroxyl group, the other is a hydrogen atom, a hydroxyl group, or a substituent other than a hydroxyl group. R ₂ , R ₃ , R ₄ may be each independently a hydrogen atom, a hydroxyl group, or a substituent other than a hydroxyl group, or R ₂ and R ₃ , or R ₃ and R ₄ may combine to form an aromatic ring. Good)) can be used.
In the above formula (2), as a compound in which R ₂ and R ₃ , or R ₃ and R ₄ are combined to form an aromatic ring, the following general formula (3)

(In the above formula (3), one of R ₁ and R ₇ is a hydroxyl group, and when one is a hydroxyl group, the other is hydrogen, a hydroxyl group, or a substituent other than a hydroxyl group. R ₂ , R ₃ , R ₄ , R ₅ , and R ₆ are each independently hydrogen, a hydroxyl group, or a substituent other than a hydroxyl group).

  Examples of the compound (G) used in the present invention include catechol, pyrogallol, gallic acid, gallic acid ester, 1,2-dihydroxynaphthalene, 2,3-dihydroxynaphthalene, and derivatives thereof. These compounds may be used alone or in combination.

  Among these, 1,2-dihydroxynaphthalene, 2,3-dihydroxynaphthalene, and derivatives thereof, in which the mother nucleus is a naphthalene ring from the viewpoint of easy control of fluidity and curability and low volatility, More preferred.

  The compounding amount of the compound (G) is 0.01% by weight or more and 1% by weight or less, preferably 0.03% by weight or more and 0.8% by weight or less, particularly preferably 0.05% by weight in the total epoxy resin composition. % Or more and 0.5% by weight or less. If it exists in the said range, the viscosity characteristic by the synergistic effect with a silane coupling agent (F) and a flow characteristic will be acquired. Furthermore, the physical properties of the cured product are excellent and can be preferably used as an epoxy resin composition.

  The epoxy resin composition for semiconductor encapsulation of the present invention contains the above-described components (A) to (G) as essential components, but in addition to this, the following other additives may be blended as necessary. Other additives include, for example, brominated epoxy resins, antimony trioxide, phosphorus compounds, metal hydroxides and other flame retardants; colorants such as carbon black and bengara, low stresses such as silicone oil, silicone rubber, and synthetic rubber Agents: Antioxidants such as bismuth oxide hydrate.

  The epoxy resin composition for semiconductor encapsulation of the present invention is obtained by mixing the components (A) to (G). Specifically, after mixing the components (A) to (G) and other additives using a mixer or the like, the mixture is heated and kneaded using a heating kneader, a hot roll, an extruder, etc., followed by cooling, It is obtained by grinding.

  A semiconductor device can be manufactured by sealing an electronic component such as a semiconductor element using the epoxy resin composition for semiconductor sealing of the present invention. In order to seal an electronic component such as a semiconductor element, it can be cured and molded by a conventional molding method such as transfer molding, compression molding, injection molding, or the like.

  EXAMPLES Hereinafter, although an Example demonstrates this invention concretely, this invention is not limited to these. The blending ratio is parts by weight.

<Example A>
(Example a1)
In Example a1, the following raw materials were used.
-Epoxy resin of the following general formula (4) (phenol aralkyl type epoxy resin having a biphenylene skeleton) [manufactured by Nippon Kayaku, NC3000P, softening point 58 ° C, epoxy equivalent 273]
7.36 parts by weight

(N is an average value and is a positive number from 1 to 3)
Phenol resin of formula (5) (phenol aralkyl resin having a phenylene skeleton [Mitsui Chemicals, XLC-4L, softening point 65 ° C., hydroxyl equivalent 174]
4.69 parts by weight

(N is an average value and is a positive number from 1 to 3)
1,8-diazabicyclo (5,4,0) undecene-7 (hereinafter referred to as “DBU”)
0.20 parts by weight, spherical fused silica (average particle size 30.0 μm) 87.00 parts by weight, oxidized polyethylene wax 1 (drop point 120 ° C., acid value 20 mg KOH / g, number average molecular weight 2000, density 0.98 g / cm ³ , average particle size 45 μm, particle size 106 μm or larger particles 0.0% by weight, high density polyethylene polymer oxide)
0.10 parts by weight • γ-glycidylpropyltrimethoxysilane 0.30 parts by weight • 2,3-dihydroxynaphthalene (reagent) 0.05 parts by weight • carbon black 0.30 parts by weight

  After mixing the above raw materials using a mixer, the kneaded product sheet obtained by kneading 20 times using a biaxial roll having surface temperatures of 95 ° C. and 25 ° C. is cooled and pulverized to obtain an epoxy resin composition and did. The characteristics of the obtained epoxy resin composition were evaluated by the following methods. The results are shown in Table 1.

(Evaluation method)
Spiral flow: Measurement was performed using a spiral flow measurement mold according to EMMI-1-66 at a mold temperature of 175 ° C., an injection pressure of 6.9 MPa, and a curing time of 120 seconds. The unit is cm.

  Metal wire deformation rate: 160 pLQFP (CuL / F, package outer dimensions: 24 mm × 24 mm × 1.4 mm thickness) with a mold temperature of 175 ° C., injection pressure of 9.6 MPa, curing time of 70 seconds using a low-pressure transfer automatic molding machine , Pad size: 8.5 mm × 8.5 mm, chip size 7.4 mm × 7.4 mm). The molded 160 pLQFP package was observed with a soft X-ray fluoroscope, and the deformation rate of the gold wire was expressed as a ratio of (flow rate) / (gold wire length). The criterion was ○ for less than 5% and x for 5% or more.

  Continuous formability: 80pQFP (CuL / F, package external dimensions: 14mm x 20mm x 2mm thickness, pad size, with a mold temperature of 175 ° C, injection pressure of 9.6MPa, curing time of 70 seconds, using a low-pressure transfer automatic molding machine : 6.5 mm × 6.5 mm, chip size 6.0 mm × 6.0 mm) was continuously molded up to 500 shots. The judgment criteria were “good” for continuous molding up to 500 shots without any problem such as unfilling, and “x” for the others.

  Molded Product Appearance and Mold Dirt: Dirt was evaluated visually for the package and mold after 500 shots in the continuous molding. The package appearance judgment and the mold contamination standard are indicated by “x” when dirty and by “◯” when not dirty up to 500 shots.

  Solder reflow resistance: The package molded in the above-described evaluation of continuous formability is post-cured at 175 ° C. for 8 hours, and the resulting package is humidified at 85 ° C. and 85% relative humidity for 168 hours, followed by IR reflow treatment (260 (According to JEDEC Level 1 conditions). The package was observed with a microscope, and the crack generation rate [(crack generation rate) = (number of external crack generation packages) / (total number of packages) × 100] was calculated. Units%. The number of packages evaluated was 20. Moreover, the adhesion state of the semiconductor element and the epoxy resin composition interface was observed with an ultrasonic flaw detector. The number of packages evaluated was 20. The criteria for determining the solder reflow resistance were a crack occurrence rate of 0% and no peeling: ○, and those where cracks or peeling occurred occurred as x.

(Examples a2 to a23, comparative examples a1 to a9)
Each component was mix | blended in the ratio shown in Table 1, Table 2, and Table 3, the epoxy resin composition was obtained like Example a1, and it evaluated similarly to Example a1. The results are shown in Table 1, Table 2, and Table 3.
Components used in Examples other than Example a1 are shown below.

-Phenol resin (phenol aralkyl resin having a biphenylene skeleton) represented by the following formula (6) [Maywa Kasei Co., Ltd., MEH7851SS, softening point 67 ° C, hydroxyl group equivalent 203]

(N is an average value and is a positive number from 1 to 3)
-Epoxy resin (biphenyl type epoxy resin) of the following formula (7) [manufactured by Jaban Epoxy Resin Co., Ltd., YX-4000H, melting point 105 ° C., epoxy equivalent 191]

Oxidized polyethylene wax 2 (drop point 105 ° C., acid value 20 mg KOH / g, number average molecular weight 1100, density 0.97 g / cm ³ , average particle size 45 μm, particle size 106 μm or more, 0.0% by weight, low pressure polymerization method Polyethylene wax oxide manufactured by
Oxidized polyethylene wax 3 (drop point 135 ° C., acid value 25 mgKOH / g, number average molecular weight 3000, density 0.99 g / cm ³ , average particle size 40 μm, particle size 106 μm or more, 0.0% by weight, high density polyethylene Polymer oxide)
Oxidized polyethylene wax 4 (drop point 110 ° C., acid value 12 mg KOH / g, number average molecular weight 1200, density 0.97 g / cm ³ , average particle diameter 50 μm, particle diameter 106 μm or more, 0.0% by weight, high density polyethylene Polymer oxide)

Oxidized polyethylene wax 5 (drop point 110 ° C., acid value 45 mg KOH / g, number average molecular weight 2000, density 0.97 g / cm ³ , average particle size 45 μm, particle size 106 μm or more, 0.0% by weight, high pressure polymerization method Polyethylene wax oxide manufactured by
Oxidized polyethylene wax 6 (drop point 110 ° C., acid value 20 mgKOH / g, number average molecular weight 750, density 0.98 g / cm ³ , average particle size 45 μm, particle size 106 μm or more, 0.0% by weight, high density polyethylene Polymer oxide)
Oxidized polyethylene wax 7 (drop point 130 ° C., acid value 20 mg KOH / g, number average molecular weight 4500, density 0.99 g / cm ³ , average particle size 45 μm, particle size 106 μm or more, 0.0% by weight, high pressure polymerization method Polyethylene wax oxide manufactured by

Oxidized polyethylene wax 8 (drop point 110 ° C., acid value 20 mg KOH / g, number average molecular weight 1100, density 0.95 g / cm ³ , average particle size 45 μm, particle size 106 μm or more, 0.0% by weight, low pressure polymerization method Polyethylene wax oxide manufactured by
Oxidized polyethylene wax 9 (dropping point 110 ° C., acid value 25 mg KOH / g, number average molecular weight 2000, density 1.02 g / cm ³ , average particle size 45 μm, particle size 106 μm or more, 0.0% by weight, high density polyethylene Polymer oxide)
Oxidized polyethylene wax 10 (drop point 120 ° C., acid value 20 mgKOH / g, number average molecular weight 2000, density 0.98 g / cm ³ , average particle size 30 μm, particle size 106 μm or more, 0.0% by weight, high density polyethylene Polymer oxide)
Oxidized polyethylene wax 11 (drop point 120 ° C., acid value 20 mg KOH / g, number average molecular weight 2000, density 0.98 g / cm ³ , average particle size 60 μm, particle size 106 μm or more, 0.0% by weight, high density polyethylene Polymer oxide)

Polyethylene wax 1 (drop point 135 ° C., acid value 0 mg KOH / g, number average molecular weight 5500, density 0.93 g / cm ³ , average particle size 45 μm, particle size 106 μm or more, 0.0% by weight, by low pressure polymerization method Manufactured polyethylene wax)
Polyethylene wax 2 (drop point 115 ° C., acid value 0 mg KOH / g, number average molecular weight 1800, density 0.93 g / cm ³ , average particle diameter 45 μm, particle diameter 106 μm or more, 0.0% by weight, by high pressure polymerization method Manufactured polyethylene wax)

・ 1,2-Dihydroxynaphthalene (reagent)
・ Catechol (reagent)
・ Pyrogallol (reagent)
・ 1,6-Dihydroxynaphthalene (reagent)
・ Resorcinol (reagent)

  In any of Examples a1 to a23, good results were obtained in the spiral flow and the gold wire deformation rate, it was confirmed that the epoxy resin composition for semiconductor encapsulation was excellent in fluidity, and further in continuous moldability. Also confirmed to be excellent. Further, no contamination was observed on the surface of the molded product and the surface of the mold, and it was confirmed that the molded product was excellent in releasability from the mold, and was also excellent in solder reflow resistance.

  On the other hand, in the comparative example a1 in which the epoxy resin represented by the general formula (4) and the phenol resin represented by the general formula (6) are not used, it is not possible to achieve low moisture absorption and low stress at high temperatures. The solder reflow resistance was inferior.

  Further, in Comparative Examples a2 and a3 in which the oxidized polyethylene wax (E1) was not used, the continuous moldability (productivity) was deteriorated, and the appearance of the molded product, the contamination of the mold, and the solder reflow resistance were inferior. In Comparative Example a4 in which the blending amount of the oxidized polyethylene wax (E1) is insufficient, the releasability is lowered, resulting in inferior continuous moldability and solder reflow resistance. In Comparative Example a5 in which the blending amount of the oxidized polyethylene wax (E1) is excessive, the excess component bleeds to the interface with the member and the surface of the cured product, thereby causing contamination on the mold surface and further on the surface of the molded product. confirmed. Furthermore, the solder reflow resistance was inferior.

  Moreover, in Comparative Examples a6, a8 and a9 in which the compound (G) was not added, the fluidity of the resin composition was lowered, and the gold wire deformation rate was deteriorated. Furthermore, in Comparative Examples a8 and a9, the solder reflow resistance was inferior. In Comparative Example a7 in which the compounding amount of compound (G) is excessive, continuous moldability (productivity) deteriorates due to a decrease in the curability of the resin composition, and contamination is confirmed on the surface of the molded product and the mold surface. did.

  As described above, the epoxy resin composition for semiconductor encapsulation of the present invention is excellent in balance of fluidity, mold release property, and continuous moldability, and further excellent in solder reflow resistance by using this resin composition. It has been confirmed that a semiconductor device package can be provided.

<Example B>
(Example b1)
In Example b1, the following raw materials were used.
-Epoxy resin of the above formula (4) (phenol aralkyl type epoxy resin having a biphenylene skeleton) [manufactured by Nippon Kayaku, NC3000P, softening point 58 ° C, epoxy equivalent 273]
7.36 parts by weight of phenol resin of the above formula (5) (phenol aralkyl resin having a phenylene skeleton [manufactured by Mitsui Chemicals, XLC-4L, softening point 65 ° C., hydroxyl group equivalent 174]
4.69 parts by weight. DBU 0.20 part by weight. Spherical fused silica (average particle size 30.0 .mu.m) 87.00 parts by weight. Glycerol trimontanate (manufactured by Clariant Japan Co., Ltd., Recolve WE4, dropping point 82.degree. , Acid value 25 mgKOH / g, average particle size 45 μm, particle size 106 μm or more particles 0.0 wt%) 0.10 parts by weight · γ-glycidylpropyltrimethoxysilane 0.30 parts by weight · 2,3-dihydroxynaphthalene ( Reagent) 0.05 part by weight, carbon black 0.30 part by weight

  The above raw materials are mixed using a mixer, then kneaded 20 times using biaxial rolls having surface temperatures of 95 ° C. and 25 ° C., and the resulting kneaded material sheet is cooled and pulverized to obtain an epoxy resin composition. It was. The properties of the obtained epoxy resin composition were evaluated in the same manner as in Example A. The results are shown in Table 4.

(Examples b2-b15, comparative examples b1-b8)
Each component was mix | blended in the ratio shown in Table 4, Table 5, and Table 6, the epoxy resin composition was obtained like Example b1, and it evaluated similarly to Example b1. The results are shown in Table 4, Table 5, and Table 6.
The components used other than the above are shown below.
・ Glycerin trimellisin ester (drop point 95 ° C., acid value 30 mg KOH / g, average particle size 45 μm, particle size 0.06% by weight of 106 μm or more)
・ Glycerin tribehenate (drop point 80 ° C., acid value 15 mgKOH / g, average particle size 45 μm, particle size 0.06% by weight of 106 μm or more)
・ Glycerin monostearate (Riken Vitamin Co., Ltd., Riquemar S-100, dropping point 65 ° C., acid value 2 mgKOH / g, average particle size 45 μm, particle size 106 μm or more 0.0% by weight)

  In any of Examples b1 to b15, good results were obtained in the spiral flow and the gold wire deformation rate, and it was confirmed that the epoxy resin composition for semiconductor encapsulation was excellent in fluidity, and further in continuous moldability. Also confirmed to be excellent. Further, no contamination was observed on the surface of the molded product and the surface of the mold, and it was confirmed that the molded product was excellent in releasability from the mold, and was also excellent in solder reflow resistance.

  On the other hand, in the comparative example b1 in which the epoxy resin represented by the general formula (4) and the phenol resin represented by the general formula (6) are not used, it is not possible to achieve low moisture absorption and low stress at high temperatures. The solder reflow resistance was inferior.

  Further, in Comparative Example b2 in which glycerin trifatty acid ester (E2) was not used, the continuous moldability (productivity) was deteriorated, and the molded product appearance, mold contamination, and solder reflow resistance were inferior. In Comparative Example b3 in which the blending amount of glycerin trifatty acid ester (E2) is insufficient, continuous moldability and solder reflow resistance were inferior due to a decrease in releasability. In Comparative Example b4 in which the blending amount of glycerin trifatty acid ester (E) is excessive, the excess component bleeds to the interface with the member and the surface of the cured product, thereby causing contamination on the mold surface and further on the surface of the molded product. It was confirmed. Furthermore, the solder reflow resistance was inferior.

  Further, in Comparative Examples b5, b7 and b8 to which no compound (G) was added, the fluidity of the resin composition was lowered, and the gold wire deformation rate was deteriorated. Further, in Comparative Examples b7 and b8, the solder reflow resistance was inferior. In Comparative Example b6 in which the compounding amount of compound (G) is excessive, continuous moldability (productivity) deteriorates due to a decrease in the curability of the resin composition, and contamination is confirmed on the surface of the molded product and the mold surface. did.

  As described above, the epoxy resin composition for semiconductor encapsulation of the present invention is excellent in balance of fluidity, mold release property, and continuous moldability, and further excellent in solder reflow resistance by using this resin composition. It has been confirmed that a semiconductor device package can be provided.

<Example C>
(Example c1)
In Example c1, the following raw materials were used.
-Epoxy resin of the above formula (4) (phenol aralkyl type epoxy resin having a biphenylene skeleton) [manufactured by Nippon Kayaku, NC3000P, softening point 58 ° C, epoxy equivalent 273]
7.36 parts by weight of phenol resin of the above formula (5) (phenol aralkyl resin having a phenylene skeleton [manufactured by Mitsui Chemicals, XLC-4L, softening point 65 ° C., hydroxyl group equivalent 174]
4.69 parts by weight. DBU 0.20 parts by weight. Spherical fused silica (average particle size 30.0 .mu.m) 87.00 parts by weight. Oxidized paraffin wax 1 (softening point 100.degree. C., acid value 15 mg KOH / g, average particle size 45 .mu.m. , 0.0% by weight of particles having a particle size of 106 μm or more)
0.10 parts by weight • γ-glycidylpropyltrimethoxysilane 0.30 parts by weight • 2,3-dihydroxynaphthalene (reagent) 0.05 parts by weight • carbon black 0.30 parts by weight

  After mixing the above raw materials using a mixer, the kneaded product sheet obtained by kneading 20 times using a biaxial roll having surface temperatures of 95 ° C. and 25 ° C. is cooled and pulverized to obtain an epoxy resin composition and did. The properties of the obtained epoxy resin composition were evaluated in the same manner as in Example A. The results are shown in Table 7.

(Examples c2 to c14, comparative examples c1 to c8)
Each component was mix | blended in the ratio shown in Table 7, Table 8, and Table 9, the epoxy resin composition was obtained like Example c1, and it evaluated similarly to Example c1. The results are shown in Table 7, Table 8, and Table 9.
The components used other than the above are shown below.
Oxidized paraffin wax 2 (softening point 105 ° C., acid value 25 mg KOH / g, average particle size 45 μm, particle size 106 μm or more 0.0% by weight)
Paraffin wax (softening point 70 ° C., acid value 0 mg KOH / g, average particle size 45 μm, particle size 106 μm or more, 0.0% by weight, non-oxidized product)

  In any of Examples c1 to c14, good results were obtained in spiral flow and gold wire deformation rate, and it was confirmed that the epoxy resin composition for semiconductor encapsulation was excellent in fluidity, and further in continuous moldability. Also confirmed to be excellent. Further, no contamination was observed on the surface of the molded product and the surface of the mold, and it was confirmed that the molded product was excellent in releasability from the mold, and was also excellent in solder reflow resistance.

  On the other hand, in the comparative example c1 which does not use the epoxy resin represented by the general formula (4) and the phenol resin represented by the general formula (6), it is not possible to achieve low moisture absorption and low stress at high temperatures. The solder reflow resistance was inferior.

  Further, in Comparative Example c2 in which the oxidized paraffin wax (E3) was not used, the continuous moldability (productivity) was deteriorated, and the molded product appearance, mold contamination, and solder reflow resistance were inferior. In Comparative Example c3 in which the blending amount of the oxidized paraffin wax (E3) is insufficient, the releasability is lowered, resulting in inferior continuous moldability and solder reflow resistance. In Comparative Example c4 in which the blending amount of the oxidized paraffin wax (E3) is excessive, the excess component bleeds to the interface with the member and the surface of the cured product, thereby causing contamination on the mold surface and further on the surface of the molded product. confirmed. Furthermore, the solder reflow resistance was inferior.

  Moreover, in Comparative Examples c5, c7 and c8 to which no compound (G) was added, the fluidity of the resin composition was lowered, and the gold wire deformation rate was deteriorated. In Comparative Examples c7 and c8, the solder reflow resistance was inferior. In Comparative Example c6 in which the compounding amount of compound (G) is excessive, continuous moldability (productivity) is deteriorated due to a decrease in the curability of the resin composition, and contamination is confirmed on the surface of the molded product and the mold surface. did.

  As described above, the epoxy resin composition for semiconductor encapsulation of the present invention is excellent in balance of fluidity, mold release property, and continuous moldability, and further excellent in solder reflow resistance by using this resin composition. It has been confirmed that a semiconductor device package can be provided.

  The epoxy resin composition for semiconductor encapsulation of the present invention is excellent in fluidity, releasability, continuous moldability and the like, and is also excellent in cured product characteristics such as solder reflow resistance. Therefore, it can be suitably used as a material for sealing a semiconductor element, and a semiconductor device in which the semiconductor element is sealed with the resin composition can be provided.

Claims (10)

(A) epoxy resin,
(B) phenolic resin,
(C) a curing accelerator,
(D) inorganic filler,
(E2) glycerin trifatty acid ester,
(F) a silane coupling agent, and (G) a compound in which a hydroxyl group is bonded to each of two or more adjacent carbon atoms constituting an aromatic ring,
At least one of the epoxy resin (A) and the phenol resin (B) is represented by the following general formula (1)

(In the general formula (1), R is a group selected from a hydrogen atom or an alkyl group having 1 to 4 carbon atoms, and a plurality of R may be the same or different from each other. , Glycidyl ether group or hydroxyl group, n is an average value and is a positive number of 1 to 3.)
Including a resin represented by
The total epoxy resin composition contains 0.01% by weight or more and 1% by weight or less of the glycerin trifatty acid ester (E2), and 0.01% by weight or more and 1% by weight or less of the compound (G). An epoxy resin composition for semiconductor encapsulation. 2. The epoxy resin composition for semiconductor encapsulation according to claim 1, wherein the total epoxy resin composition contains 0.01 to 0.5% by weight of the glycerin trifatty acid ester (E2). The epoxy resin composition for semiconductor encapsulation according to claim 1, wherein the total epoxy resin composition contains 0.03 wt% or more and 0.5 wt% or less of the glycerin trifatty acid ester (E2). The epoxy resin composition for semiconductor encapsulation according to any one of claims 1 to 3, wherein the total epoxy resin composition contains the compound (G) in an amount of 0.03% by weight to 0.8% by weight. The compound (G) is represented by the following general formula (2)

(In the general formula (2), one of R ₁ and R ₅ is a hydroxyl group, and when one is a hydroxyl group, the other is a hydrogen atom, a hydroxyl group, or a substituent other than a hydroxyl group. R ₂ , R ₃ , R ₄ may be each independently a hydrogen atom, a hydroxyl group, or a substituent other than a hydroxyl group, or R ₂ and R ₃ , or R ₃ and R ₄ may combine to form an aromatic ring. It is good.) The epoxy resin composition for semiconductor sealing in any one of Claims 1 thru | or 4 represented by these. The epoxy resin composition for semiconductor encapsulation according to any one of claims 1 to 5, wherein a dropping point of the glycerin trifatty acid ester (E2) is 70 ° C or higher and 120 ° C or lower. The average particle size of the glycerin trifatty acid ester (E2) is 20 µm or more and 70 µm or less, and the content ratio of particles having a particle size of 106 µm or more in the total glycerin trifatty acid ester (E2) is 0.1 wt% or less. The epoxy resin composition for semiconductor sealing in any one of 1 thru | or 6 . The epoxy resin composition for semiconductor encapsulation according to any one of claims 1 to 7 , wherein an acid value of the glycerin trifatty acid ester (E2) is 10 mgKOH / g or more and 50 mgKOH / g or less. The epoxy resin composition for semiconductor encapsulation according to any one of claims 1 to 8 , wherein the glycerin trifatty acid ester (E2) is a triester compound of glycerin and a saturated fatty acid having 24 to 36 carbon atoms. Wherein a obtained by encapsulating a semiconductor element using the epoxy resin composition for semiconductor encapsulation according to any one of claims 1 to 9.