TW202104441A - A curable hotmelt silicone composition, encapsulant, film and optical semiconductor device - Google Patents

Abstract

The present invention provides a hot-melt curable organosilicon composition which can exhibit excellent mechanical properties, particularly strength and elongation, even when being molded into a film shape or a sheet shape. The above issue is solved by a solvent-free, hot-melt curable organosilicon composition, and the solvent-free, hot-melt curable organosilicon composition includes: (A) an alkenyl group-containing organopolysiloxane, wherein at least two alkenyl groups are provided in one molecule; (B) a branched organohydrogen polysiloxane, which is 0.1 to 5 mass% with respect to the total mass of the composition, and at least two silicon atoms are bonded to hydrogen atoms in one molecule; (C) an additive represented by the average unit formula (C-1); (D) a catalyst for hydrosilylation reaction; and (E) silicon dioxide.

Description

Hot-melt curable organosilicon composition, sealant, film and optical semiconductor element

The present invention relates to a curable organosilicon composition, and more specifically, to a curable organosilicon composition for sealing, covering or bonding optical semiconductor devices. In addition, the present invention also relates to a sealant composed of such a curable organosilicon composition and an optical semiconductor element containing the sealant. In addition, the present invention also relates to a film obtained by curing the curable organosilicon composition.

The curable silicone composition is cured to form a cured product with excellent heat resistance, cold resistance, electrical insulation, weather resistance, water repellency, and transparency, so it is widely used in industrial fields. In particular, the cured product is less likely to change color than other organic materials, and its physical properties are less reduced, so it is suitable for use in optical materials.

For example, Patent Documents 1 to 3 describe a resin composition for sealing optical semiconductor devices or for optical lenses using a curable silicone resin composition. The curable silicone resin composition contains one molecule Organopolysiloxanes having two or more non-covalently bonded double bond groups, organohydrogenpolysiloxanes having two or more hydrogen atoms bonded to silicon atoms in one molecule, and catalytic amounts of platinum catalyst. In addition, Patent Documents 4 and 5 describe a hot-melt silicone resin composition, which is non-flowing at 25°C, has low surface adhesion, and is easily melted by heating. [Prior Technical Literature] [Patent Literature]

[Patent Document 1]: Japanese Patent Application Publication No. 2006-299099 [Patent Document 2]: Japanese Patent Application Publication No. 2007-246894 [Patent Document 3]: Japanese Patent Laid-Open No. 2006-324596 [Patent Document 4]: JP 2013-001794 A [Patent Document 5]: International Publication No. 2015/194158

[Problems to be solved by the invention] However, when a conventional silicone resin composition is used to produce a hot-melt film, there is a problem that the mechanical properties of the film, particularly the strength and elongation of the film are insufficient. Therefore, for example, when it is used for the formation of a film-like or sheet-like sealant and a lamination film in the manufacture of a semiconductor package, the resulting film is easily broken and its handling performance is insufficient.

The object of the present invention is to provide a hot-melt curable silicone composition that can exhibit excellent mechanical properties, especially strength and elongation, even when it is molded into a film or sheet shape. More specifically, there is provided a hot-melt curable organosilicon composition capable of forming a sheet-like or film-like sealant and a lamination film that can efficiently manufacture semiconductor packages with excellent processing performance. [Means used to solve the problem]

In order to solve the above-mentioned problems, the inventors of the present invention conducted intensive studies, and found that the solvent-free hot-melt curable silicone composition can solve the above-mentioned problems and achieved the present invention. The curable organosilicon composition includes: (A) Organopolysiloxane, which has at least two alkenyl groups in one molecule; (B) Resin-like organohydrogenpolysiloxane, which is 0.1 relative to the total mass of the composition ~ 5% by mass, with at least two silicon atoms bonded to hydrogen atoms in one molecule; (C) an additive represented by the following average unit formula (C-1): (R ¹ ₃ SiO _1/2 ) _a (R ¹ ₂ SiO _2/2 ) _b (R ¹ SiO _3/2 ) _{c In the} formula, R ¹ is the same or different organic groups containing alkyl, aryl, alkenyl, aralkyl, or epoxy groups, wherein , At least one R ¹ is an alkenyl group, and at least one R ¹ is an epoxy-containing organic group, a, b, and c are numbers satisfying the following conditions: 0 ≤ a ≤ 1.0, 0 ≤ b ≤ 1.0, 0 ≤ c <0.9, and a + b + c = 1; (D) catalyst for hydrosilylation reaction; and (E) silicon dioxide.

In one embodiment of the present invention, the component (A) contains a _{resinous organopolysiloxane containing at least one (Ar 2} SiO _2/2 ) unit.

In one embodiment of the present invention, the (B) component is represented by the following (B-1) average unit formula: (R ³ ₃ SiO _1/2 ) _a (R ³ ₂ SiO _2/2 ) _b (R ³ SiO _{3 /2} ) _c (SiO _4/2 ) _d (XO _1/2 ) _{e In the} formula, R ³ is a hydrogen atom or the same or different halogen substituted or unsubstituted monovalent hydrocarbon group, wherein at least two R ³ are A hydrogen atom, X is a hydrogen atom or an alkyl group, a, b, c, d and e are numbers satisfying the following conditions: 0 ≤ a ≤ 1.0, 0 ≤ b ≤ 1.0, 0 ≤ c ＜ 0.9, 0 ≤ d ＜ 0.5 , 0 ≤ e <0.4, a + b + c + d = 1.0, and c + d> 0.

In the above average unit formula (B-1), a can be in the range of 0.1 ≤ a ≤ 0.9, b can be in the range of 0 ≤ b ≤ 0.8, c can be in the range of 0.1 ≤ c ≤ 0.9, and d can be in the range of 0 ≤ In the range of d ≤ 0.4, e may be in the range of 0 ≤ e ≤ 0.3.

In the above average unit formula (C-1), a may be in the range of 0 ≤ a ≤ 0.9, b may be in the range of 0.1 ≤ b ≤ 0.9, and c may be in the range of 0.01 ≤ c ≤ 0.8.

(C) The content of the alkenyl group contained in the component may be 5 mol% or more of the total of ^{R 1.}

(C) The content of the epoxy group-containing organic group contained in the component may be 5 mol% or more of the sum of ^{R 1.}

In one embodiment of the present invention, the component (A) contains linear, branched, and cyclic organopolysiloxanes.

The present invention also relates to a film obtained by curing the hot-melt curable organosilicon composition of the present invention.

The present invention also relates to a sealant composed of the hot-melt curable organosilicon composition of the present invention.

The present invention also relates to an optical semiconductor device containing the sealant of the present invention.

The semiconductor device of the present invention is preferably a light emitting diode. [Effects of the invention]

The hot-melt curable silicone composition of the present invention can exhibit excellent mechanical properties, especially strength and elongation, even when it is molded into a film or sheet shape. Therefore, the hot-melt curable silicone composition of the present invention has excellent processing performance and can form a sheet-like or film-like sealant and a laminate film that can efficiently manufacture semiconductor packages.

In addition, the sealant of the present invention is formed of the hot-melt curable silicone composition of the present invention, and therefore can exhibit excellent mechanical properties, particularly strength and elongation, and as a result, excellent handling performance. Therefore, the semiconductor package can be manufactured efficiently.

Hereinafter, the present invention will be described in detail. [Hot-melt curable silicone composition]

The present invention relates to a solvent-free hot-melt curable organosilicon composition, comprising: (A) organopolysiloxane having at least two alkenyl groups in one molecule; (B) resinous organohydrogen polysiloxane Alkane, which is 0.1 to 5 mass% relative to the total mass of the composition, and has at least two silicon atoms bonded to hydrogen atoms in one molecule; (C) an additive represented by the following average unit formula (C-1): ( R ¹ ₃ SiO _1/2 ) _a (R ¹ ₂ SiO _2/2 ) _b (R ¹ SiO _3/2 ) _{c In the} formula, R ¹ is the same or different containing alkyl, aryl, alkenyl, aralkyl Or epoxy group, wherein at least one R ¹ is an alkenyl group, and at least one R ¹ is an epoxy group-containing organic group, and a, b, and c are numbers satisfying the following conditions: 0 ≤ a ≤ 1.0, 0 ≤ b ≤ 1.0, 0 ≤ c ＜ 0.9, and a + b + c = 1; (D) catalyst for hydrosilylation reaction; and (E) silicon dioxide.

The organosilicon composition of the present invention does not contain a solvent. In addition, it exhibits hot-melt properties when it is formed into a film or sheet by heat treatment. In this specification, "hot-melt" means that it is non-flowing at 25°C, but it is easy to melt by heating and exhibits fluidity characteristics. For example, the melt elastic modulus of the hot-melt silicone composition of the present invention at 100°C is in the range of 10 Pa to 1 MPa. Here, non-fluidity means that it does not flow under no load. For example, when compared to the hot-melt adhesive specified by JIS K 6863-1994 "Test Method for Softening Point of Hot-melt Adhesives" The state when the softening point is low as measured by the softening point test method of the ring and ball method. That is, the hot-melt silicone composition of the present invention preferably has a softening point higher than 25°C. In addition, the melt elastic modulus at 100°C can be measured with a flat-plate viscoelasticity meter that can control the temperature. In addition, the organosilicon composition of the present invention is a hot-melt curable organosilicon composition having both hot-melt properties and curability.

Such a hot-melt curable silicone composition of the present invention can exhibit excellent mechanical properties, particularly strength and elongation, even when it is molded into a film or sheet shape. Therefore, the hot-melt curable organosilicon composition of the present invention has excellent processing performance and can form a sealant and a laminate film that can efficiently manufacture semiconductor packages and are used in the manufacture of semiconductor packages.

Hereinafter, each component will be described in detail.

(A) Organopolysiloxane containing alkenyl groups The component (A) is an alkenyl group-containing organopolysiloxane having at least two silicon atoms bonded to an alkenyl group in one molecule, which is the main ingredient of the curable silicone composition of the present invention.

The alkenyl group contained in the component (A) may, for example, be vinyl, propenyl, butenyl, pentenyl, hexenyl, heptenyl, octenyl, nonenyl, decenyl, ten Alkenyl groups with 2 to 12 carbon atoms such as monoalkenyl and dodecenyl are preferably vinyl groups.

(A) The molecular structure of the component may, for example, be a linear structure, a partially branched linear structure, a branched structure, a cyclic structure, or a three-dimensional network structure. The component (A) can also be one organopolysiloxane having these molecular structures, or a mixture of two or more organopolysiloxanes having these molecular structures. The curable silicone composition of the present invention preferably contains both linear organopolysiloxane and resinous organopolysiloxane as component (A).

In one embodiment of the present invention, the (A) component may be: a linear organopolysiloxane represented by the following (A-1) average unit formula: R ² ₃ SiO(R ² ₂ SiO) _m SiR ² _{In the} formula 3, R ² is the same or different halogen-substituted or unsubstituted monovalent hydrocarbon group, wherein at least two R ^{2 in} a molecule are alkenyl groups, and m is an integer from 4 to 1,000; and/or is composed of (A -2) The branched organopolysiloxane represented by the average unit formula: (R ² ₃ SiO _1/2 ) _a (R ² ₂ SiO _2/2 ) _b (R ² SiO _3/2 ) _c (SiO _{4/ 2} ) _d (XO _1/2 ) _{e In the} formula, R ² is the same as above, wherein at least two R ^{2 in} a molecule are alkenyl groups, X is a hydrogen atom or an alkyl group, a, b, c, d and e It is a number that satisfies the following conditions: 0 ≤ a ≤ 1.0, 0 ≤ b ≤ 1.0, 0 ≤ c ＜ 0.9, 0 ≤ d ＜ 0.5, 0 ≤ e ＜ 0.4, a + b + c + d + e = 1.0, and c + d ＞ 0; and/or a cyclic organopolysiloxane represented by the following (A-3) average unit formula: (R ² SiO _2/2 ) _{n In the} formula, R ² is the same as above, where one At least two R ^{2 in the} molecule are alkenyl groups, and n is an integer of 3-50.

Preferably, the hot-melt curable silicone composition of the present invention contains both linear and branched organopolysiloxanes as the (A) component. More preferably, the hot-melt curable silicone composition of the present invention contains linear, branched, and cyclic organopolysiloxanes as the (A) component. In addition, the branched-chain organopolysiloxane-based resin-like organopolysiloxane means that one molecule contains at least one siloxane unit (M unit) represented _{by the general formula: R 3} SiO _1/2. The siloxane unit (D unit) represented by the formula R ₂ SiO _2/2 , the siloxane unit (T unit) represented _{by the general formula RSiO 3/2} , and the siloxane unit represented _{by the formula SiO 4/2 (} Q unit) in the T unit or Q unit organopolysiloxane.

^{As the halogen-substituted or unsubstituted monovalent hydrocarbon group of R 2} in the above formula, methyl, ethyl, propyl, isopropyl, butyl, isobutyl, tertiary butyl, pentyl, neopentyl Alkyl groups with 1 to 12 carbon atoms such as hexyl, hexyl, cyclohexyl, heptyl, octyl, nonyl, decyl, undecyl, dodecyl, etc.; phenyl, tolyl, xylyl, naphthalene C6-C20 aryl groups such as benzyl, phenethyl, phenylpropyl and other C7-20 aralkyl groups; vinyl, propenyl, butenyl, pentenyl, hexene Alkenyl, heptenyl, octenyl, nonenyl, decenyl, undecenyl, dodecenyl and other alkenyl groups with 2 to 12 carbon atoms; and halogens such as fluorine, chlorine, and bromine atoms A group in which an atom partially or completely replaces the hydrogen atom of the group. As long as the purpose of the present invention is not impaired, R ² may be an alkoxy group having a small amount of hydroxyl, methoxy, and ethoxy.

R ^{2 is} preferably selected from phenyl, alkyl or cycloalkyl having 1 to 6 carbon atoms, or alkenyl having 2 to 6 carbon atoms.

(A) The content of the alkenyl group contained in the component is not particularly limited, but it is preferable that 0.01 to 50 mol%, 0.05 to 40 mol%, or 0.09 to 32 mol% of the total amount of ^{R 2 is an alkenyl group} . In addition, the content of the alkenyl group can be determined by analysis such as Fourier transform infrared spectrophotometer (FT-IR), nuclear magnetic resonance (NMR), and the like.

The component (A) preferably contains a _{resinous organopolysiloxane containing at least one (Ar 2} SiO _2/2 ) unit.

The ratio of the T unit in the molecular structure of the resinous organopolysiloxane _{containing at least one (Ar 2} SiO _2/2 ) unit as the component (A) of the present invention is preferably 0.1 or more, more preferably 0.2 or more, more preferably 0.3 or more. In a preferred embodiment, the ratio of T units in the molecular structure of the resinous organopolysiloxane of the present invention is 0.9 or less, preferably 0.85 or less, and more preferably 0.8 or less. In another preferred embodiment, the ratio of Q units in the molecular structure of the resinous organopolysiloxane of the present invention is 0.2 or less, preferably 0.1 or less, and more preferably does not contain Q units. In addition, the ratio of the above-mentioned T unit and Q unit can be represented by the siloxane unit (M unit) represented _{by the general formula R 3} SiO _{1/2 of the resinous organopolysiloxane, and represented by the general formula R 2} SiO _2/2 . Calculate the amount of siloxane units (D units), siloxane units (T units) represented _{by the general formula RSiO 3/2} , and siloxane units (Q units) represented _{by the formula SiO 4/2.}

In the (Ar ₂ SiO _2/2 ) unit, Ar refers to an aryl group. The aryl group may be unsubstituted or substituted, preferably an aryl group having 6 to 20 carbon atoms, for example, phenyl, tolyl, xylyl, naphthyl, anthryl, phenanthryl , Pyrenyl groups, and groups in which the hydrogen atoms of these aryl groups are substituted with alkyl groups such as methyl and ethyl groups, alkoxy groups such as methoxy and ethoxy groups, and halogen atoms such as chlorine atoms and bromine atoms. It is particularly preferred that the aryl group is a phenyl group.

_{The ratio of (Ar 2} SiO _2/2 ) units in the molecular structure of the resinous organopolysiloxane as the component (A) of the present invention is preferably 0.05 or more, more preferably 0.1 or more, and still more preferably Is above 0.15, preferably above 0.2. _{In a preferred embodiment, the ratio of (Ar 2} SiO _2/2 ) units in the molecular structure of the resinous organopolysiloxane of the present invention is 0.5 or less, preferably 0.45 or less, and more preferably 0.4 or less.

In the resinous organopolysiloxane containing at least one (Ar ₂ SiO _2/2 ) unit as the component (A), it is preferable that 40 mol% or more of the monovalent hydrocarbon group bonded to the silicon atom may be aromatic More preferably, 50 mol% or more may be aryl groups, and in particular, 60 mol% or more may be aryl groups.

The component (A) resinous organopolysiloxane is preferably represented by the following average unit formula (A-4): (A-4) (R ² ₃ SiO _1/2 ) _a (R ² ₂ SiO _2/2 ) _B (Ar ₂ SiO _2/2 ) _b' (R ² SiO _3/2 ) _c (SiO _4/2 ) _d (XO _1/2 ) _{e In the} formula, R ² and Ar are the same as above, and one molecule At least two of R ² are alkenyl groups, X is a hydrogen atom or an alkyl group, R ² ₂ SiO _2/2 represents _{a unit other than Ar 2} SiO _2/2 , and a, b, b', c, d and e are satisfied Number of the following conditions: 0 ≤ a ≤ 1.0, 0 ≤ b ≤ 1.0, 0 ＜ b'≤ 1.0, 0 ≤ c ＜ 0.9, 0 ≤ d ＜ 0.5, 0 ≤ e ＜ 0.4, a + b + b'+ c + d = 1.0, and c + d> 0.

In the average unit formula (A-4), a is preferably in the range of 0 ≤ a ≤ 0.5, more preferably in the range of 0 ≤ a ≤ 0.3, most preferably in the range of 0 ≤ a ≤ 0.2, especially 0 The range of ≤ a ≤ 0.1. In the average unit formula (A-4), b is preferably in the range of 0 ≤ b ≤ 0.8, more preferably in the range of 0.1 ≤ b ≤ 0.7, especially in the range of 0.15 ≤ b ≤ 0.6. In the average unit formula (A-4), b'is preferably in the range of 0.1 ≤ b'≤ 0.7, more preferably in the range of 0.2 ≤ b'≤ 0.6, especially in the range of 0.25 ≤ b'≤ 0.5 . In the average unit formula (A-4), c is preferably in the range of 0.1 ≤ c ≤ 0.9, more preferably in the range of 0.2 ≤ c ≤ 0.85, especially in the range of 0.3 ≤ c ≤ 0.8. In the average unit formula (A-4), d is preferably in the range of 0 ≤ d ≤ 0.4, more preferably in the range of 0 ≤ d ≤ 0.3, especially in the range of 0 ≤ d ≤ 0.2. In the average unit formula (A-4), e is preferably in the range of 0 ≤ e ≤ 0.3, more preferably in the range of 0 ≤ e ≤ 0.2, especially in the range of 0 ≤ e ≤ 0.1.

Based on the total mass of the composition, the curable silicone composition of the present invention preferably contains 10% by mass or more, more preferably 20% by mass or more, more preferably 30% by mass or more, and still more preferably _{A resinous organopolysiloxane containing at least one (Ar 2} SiO _2/2 ) unit at 40% by mass or more is used as the (A) component. In a preferred embodiment, based on the total mass of the composition, the curable silicone composition of the present invention contains 90% by mass or less, preferably 80% by mass or less, and more preferably 70% by mass or less. Resin-like organopolysiloxane with at least one (Ar ₂ SiO _{2/2) unit.}

Based on the total mass of the composition of the present invention, it may contain preferably 30% by mass or more, more preferably 40% by mass or more, still more preferably 50% by mass or more, and most preferably 60% by mass or more (A) Component, and preferably 90% by mass or less, more preferably 85% by mass or less, especially 80% by mass or less (A) component may be included.

(B) Resin-like organohydrogen polysiloxane (B) Resin-like organohydrogenpolysiloxane (ie, branched organohydrogenpolysiloxane) having at least two silicon atoms bonded to hydrogen atoms in one molecule of the component is used as a curable organic hydrosilylation reaction curing type The crosslinking agent of the silicon composition functions. Preferably, the component (B) is a resinous organohydrogenpolysiloxane containing silicon atoms bonded to hydrogen atoms at least at both ends of the molecular chain. The component (B) may use only one type of organopolysiloxane, or two or more types of organopolysiloxanes in combination.

It is preferable that at least the silicon atoms of the component (B) are bonded to hydrogen atoms at least at both ends of the molecular chain. In addition, the side chains of the molecular chain may contain silicon atoms bonded to hydrogen atoms, or only at both ends of the molecular chain. Contains silicon atoms bonded to hydrogen atoms. Examples of the group bonded to the silicon atom other than the hydrogen atom in the component (B) include methyl, ethyl, propyl, isopropyl, butyl, isobutyl, tertiary butyl, and pentyl. Alkyl, neopentyl, hexyl, cyclohexyl, heptyl, octyl, nonyl, decyl, undecyl, dodecyl and other C1-C12 alkyl groups; phenyl, tolyl, di Aryl groups with 6 to 20 carbon atoms such as tolyl and naphthyl; aralkyl groups with 7 to 20 carbon atoms such as benzyl, phenethyl, and phenylpropyl; and halogens such as fluorine, chlorine, and bromine atoms A group in which an atom partially or completely replaces the hydrogen atom of the group. In addition, as long as the object of the present invention is not impaired, the silicon atom in the component (B) may have a small amount of alkoxy groups such as hydroxyl, methoxy, and ethoxy.

In one embodiment of the present invention, it may be a resinous organohydrogenpolysiloxane represented by the following (B-1) average unit formula: (R ³ ₃ SiO _1/2 ) _a (R ³ ₂ SiO _2/2 ) _B (R ³ SiO _3/2 ) _c (SiO _4/2 ) _d (XO _1/2 ) _{e In the} formula, R ³ is a hydrogen atom or the same or different halogen substituted or unsubstituted monovalent hydrocarbon group, wherein , At least two R ³ are hydrogen atoms, X is a hydrogen atom or an alkyl group, a, b, c, d and e are numbers satisfying the following conditions: 0 ≤ a ≤ 1.0, 0 ≤ b ≤ 1.0, 0 ≤ c ＜ 0.9, 0 ≤ d <0.5, 0 ≤ e <0.4, a + b + c + d = 1.0, and c + d> 0.

^{As the halogen-substituted or unsubstituted monovalent hydrocarbon group of R 3} in the above formula B-1, methyl, ethyl, propyl, isopropyl, butyl, isobutyl, tertiary butyl, and pentyl can be exemplified , Neopentyl, hexyl, cyclohexyl, heptyl, octyl, nonyl, decyl, undecyl, dodecyl and other alkyl groups with 1 to 12 carbon atoms; phenyl, tolyl, xylene Aryl groups with 6 to 20 carbon atoms, such as benzyl, naphthyl, etc.; aralkyl groups with 7 to 20 carbon atoms, such as benzyl, phenethyl, phenylpropyl, etc.; vinyl, propenyl, butenyl, pentenyl, etc. , Hexenyl, heptenyl, octenyl, nonenyl, decenyl, undecenyl, dodecenyl and other alkenyl groups with 2 to 12 carbon atoms; and use of fluorine, chlorine, bromine, etc. A group in which a halogen atom such as an atom partially or completely replaces the hydrogen atom of the group. As long as the purpose of the present invention is not impaired, R ³ may be an alkoxy group having a small amount of hydroxyl, methoxy, and ethoxy.

In the above formula B-1, a is preferably in the range of 0.1 ≤ a ≤ 0.9, more preferably in the range of 0.2 ≤ a ≤ 0.8, particularly in the range of 0.4 ≤ a ≤ 0.7. In the above formula B-1, b is preferably in the range of 0 ≤ b ≤ 0.8, more preferably in the range of 0 ≤ b ≤ 0.5, especially in the range of 0 ≤ b ≤ 0.2. In the above formula B-1, c is preferably in the range of 0.1 ≤ c ≤ 0.9, more preferably in the range of 0.2 ≤ c ≤ 0.7, especially in the range of 0.3 ≤ c ≤ 0.5. In the above formula B-1, d is preferably in the range of 0 ≤ d ≤ 0.4, more preferably in the range of 0 ≤ d ≤ 0.3, especially in the range of 0 ≤ d ≤ 0.2. In the above formula B-1, e is preferably in the range of 0 ≤ e ≤ 0.3, more preferably in the range of 0 ≤ e ≤ 0.2, especially in the range of 0 ≤ e ≤ 0.1.

Based on the total mass of the composition of the present invention, the component (B-1) is contained in the hot-melt curable silicone composition of the present invention in an amount of 0.1 to 5% by mass. Based on the total mass of the composition of the present invention, component (B) is preferably contained in an amount of 0.5% by mass or more, more preferably 1% by mass or more in the hot-melt curable silicone composition of the present invention Among them, for example, it is contained in the hot-melt curable silicone composition of the present invention in an amount of 4.5% by mass or less.

In one embodiment of the present invention, with respect to the component (B), the silicon atom in the component (A) is bonded to an alkenyl group by 1 mol, and the silicon atom in this component may preferably be bonded to a hydrogen atom from 0.001 to 1 mol. The amount of 5 mol is more preferably the amount of 0.01 to 2 mol, especially the amount of 0.05 to 1 mol.

In addition to the above-mentioned (B) component, the hot-melt curable silicone composition may also contain organohydrogenpolysiloxane as a crosslinking agent for the hydrosilylation-curable curable silicone composition as (B ')ingredient. As such (B') component, preferably, a linear organohydrogenpolysiloxane is used. The component (B’) can use only one type of organopolysiloxane, or two or more types of organopolysiloxanes in combination.

It is preferable that at least the silicon atoms containing the (B') component at both ends of the molecular chain are bonded with hydrogen atoms. In addition, the side chains of the molecular chain may contain silicon atoms bonded with hydrogen atoms, or only at both ends of the molecular chain. Contains silicon atoms bonded to hydrogen atoms. Examples of the group bonded to the silicon atom other than the hydrogen atom in the component (B) include methyl, ethyl, propyl, isopropyl, butyl, isobutyl, tertiary butyl, and pentyl. Alkyl, neopentyl, hexyl, cyclohexyl, heptyl, octyl, nonyl, decyl, undecyl, dodecyl and other C1-C12 alkyl groups; phenyl, tolyl, di Aryl groups with 6 to 20 carbon atoms such as tolyl and naphthyl; aralkyl groups with 7 to 20 carbon atoms such as benzyl, phenethyl, and phenylpropyl; and halogens such as fluorine, chlorine, and bromine atoms A group in which an atom partially or completely replaces the hydrogen atom of the group. In addition, as long as the object of the present invention is not impaired, the silicon atom in the component (B') may have a small amount of alkoxy groups such as hydroxyl groups, methoxy groups, and ethoxy groups.

In an embodiment of the present invention, the (B') component may be the average composition formula of (B-2): (R ³ ₃ SiO _1/2 ) _a (R ³ ₂ SiO _2/2 ) _b (XO _{1/ 2} ) _e (where R ³ and X are the same as above, a, b and e are numbers satisfying the following conditions: 0 ≤ a ≤ 1.0, 0 ≤ b ≤ 1.0, 0 ≤ e ＜ 0.4, and a + b = 1.0. Represents the linear organic hydrogen polysiloxane.

In one embodiment of the present invention, the (B') component can be represented by the following structural formula: [HR ⁴ ₂ SiO _1/2 ] ₂ [R ⁴ ₂ SiO _2/2 ] _{y is} represented, where R ⁴ is the same Or a different halogen-substituted or unsubstituted monovalent hydrocarbon group, y is 1-100, preferably a number in the range of 1-10. Halogen substituted or unsubstituted monovalent hydrocarbon group of R ^4, R groups may be used the same as described in ³ groups.

Based on the total mass of the composition of the present invention, the component (B') may preferably be 1% by mass or more, more preferably 5% by mass or more, most preferably 10% by mass or more, especially 15% by mass The above amount is contained in the hot-melt curable silicone composition of the present invention, and may preferably be 50% by mass or less, more preferably 40% by mass or less, especially 30% by mass or less The amount is included in the hot-melt curable silicone composition of the present invention.

Regarding the total content of (B) component and (B'), relative to 1 mol of silicon atom-bonded alkenyl group in component (A), silicon atom-bonded hydrogen atom in this component may preferably be 0.1 to The amount of 10 mol is more preferably the amount of 0.5 to 5 mol, especially the amount of 0.5 to 1.5 mol. In addition, based on the total mass of the composition of the present invention, the total content of (B) component and (B') may preferably be 1 mass% or more, more preferably 5 mass% or more, and most preferably 10 It is contained in the hot-melt curable organosilicon composition of the present invention in an amount of at least 15% by mass, and more preferably at less than 50% by mass, and more preferably at 40% by mass. Hereinafter, it is contained in the hot-melt curable silicone composition of the present invention, particularly in an amount of 30% by mass or less.

(C) Additive The additive as the component (C) of the present invention is a siloxane compound represented by the following (C-1) average unit formula: (R ¹ ₃ SiO _1/2 ) _a (R ¹ ₂ SiO _2/2 ) _B (R ¹ SiO _3/2 ) _{c In the} formula, R ¹ is the same or different organic groups or alkoxy groups containing alkyl, aryl, alkenyl, aralkyl, or epoxy groups, wherein, At least one R ¹ is an alkenyl group, and at least one R ¹ is an epoxy-containing organic group, a, b, and c are numbers satisfying the following conditions: 0 ≤ a ≤ 1.0, 0 ≤ b ≤ 1.0, 0 ≤ c <0.9, and a + b + c = 1. That is, the component (C) contains at least one alkenyl group and at least one epoxy group-containing organic group bonded to a silicon atom.

In this specification, the "epoxy group-containing group" can be exemplified by glycidyl groups such as 2-glycidoxyethyl, 3-glycidoxypropyl, 4-glycidoxybutyl, etc. Oxyalkyl; 2-(3,4-epoxycyclohexyl)-ethyl, 3-(3,4-epoxycyclohexyl)-propyl and other epoxycycloalkylalkyls; 3,4-cyclic An epoxyalkyl group such as oxybutyl and 7,8-epoxyoctyl group is preferably a glycidoxyalkyl group, and particularly preferably a 3-glycidoxypropyl group.

In this specification, "alkoxy" is, for example, methoxy, ethoxy, butoxy, phenoxy, pentoxy, allyloxy, cyclohexyloxy, benzyloxy, naphthoxy, The acetoxy group and the like are preferably methoxy group and ethoxy group, and particularly preferably methoxy group.

The alkenyl group contained in the component (C) may, for example, be vinyl, allyl, butenyl, pentenyl, hexenyl, heptenyl, octenyl, nonenyl, decenyl, Alkenyl groups having 2 to 12 carbon atoms such as undecenyl and dodecenyl are preferably vinyl groups.

^{R 1 in the} above formula C-1 is preferably selected from an alkyl group having 1 to 12 carbon atoms, an aryl group having 6 to 20 carbon atoms, or an aralkyl group having 7 to 20 carbon atoms. ^{Specifically, as R 1 of the} above formula C-1, methyl, ethyl, propyl, butyl, pentyl, hexyl, heptyl, octyl, nonyl, decyl, undecyl, Alkyl groups such as dodecyl; vinyl, propenyl, butenyl, pentenyl, hexenyl, heptenyl, octenyl, nonenyl, decenyl, undecenyl, dodecene Alkenyl groups such as phenyl; phenyl, tolyl, xylyl, naphthyl, anthryl, phenanthryl, pyrenyl and other aryl groups; naphthyl ethyl, naphthyl propyl, anthracene ethyl, phenanthryl ethyl, pyrene ethyl, etc Aralkyl group; and the hydrogen of the aryl group or aralkyl group is partially or completely replaced with alkyl groups such as methyl and ethyl groups, alkoxy groups such as methoxy and ethoxy groups, and halogen atoms such as chlorine atoms and bromine atoms The atom group is preferably a methyl group, a vinyl group, or a phenyl group.

In the above formula C-1, a is preferably in the range of 0 ≤ a ≤ 0.9, more preferably in the range of 0 ≤ a ≤ 0.5, particularly in the range of 0 ≤ a ≤ 0.3. In the above formula C-1, b is preferably in the range of 0.1 ≤ b ≤ 0.9, more preferably in the range of 0.2 ≤ b ≤ 0.8, especially in the range of 0.25 ≤ b ≤ 0.7. In the above formula C-1, c is preferably in the range of 0.01 ≤ c ≤ 0.8, more preferably in the range of 0.1 ≤ c ≤ 0.7, especially in the range of 0.2 ≤ c ≤ 0.6.

The alkenyl group content of component (C) contained is not particularly limited, for example, less than 1 mole% of the sum of R ^1, preferably 5 mole% or more, more preferably 8 mole% or more, And, for example, it is 40 mol% or less, preferably 30 mol% or less, and more preferably 30 mol% or less. In addition, the content of the alkenyl group can be determined by analysis such as Fourier transform infrared spectrophotometer (FT-IR), nuclear magnetic resonance (NMR), and the like.

(C) The content of the epoxy group-containing organic group contained in the component is not particularly limited. For example, it is ^{1 mol% or more of the sum of R 1} , preferably 5 mol% or more, and more preferably 10 Mole% or more, and for example, 50 mole% or less, preferably 40 mole% or less, and more preferably 35 mole% or less. In addition, the content of the epoxy group-containing organic group can be determined by analysis such as Fourier transform infrared spectrophotometer (FT-IR), nuclear magnetic resonance (NMR), and the like.

Based on the total mass of the composition of the present invention, component (C) may preferably be 0.01% by mass or more, more preferably 0.1% by mass or more, most preferably 0.3% by mass or more, especially 0.5% by mass or more The amount is contained in the hot-melt curable silicone composition of the present invention, and may preferably be contained in an amount of 20% by mass or less, more preferably 15% by mass or less, and most preferably in an amount of 10% by mass or less In the hot-melt curable organosilicon composition of the present invention.

(D) Catalyst for Hydrosilylation Reaction (D) The catalyst for component hydrosilylation reaction is a catalyst for accelerating the curing of the hot-melt curable organosilicon composition of the present invention. Examples of such (D) component include chloroplatinic acid, an alcohol solution of chloroplatinic acid, complexes of platinum and olefins, platinum and 1,3-divinyl-1,1,3,3-tetramethyl Palladium catalysts such as complexes of disiloxane, platinum-supported powders, and palladium catalysts such as tetrakis(triphenylphosphine)palladium, palladium black, and mixtures with triphenylphosphine; rhodium catalysts can be cited In particular, platinum-based catalysts are preferred.

The compounding amount of (D) component is the catalytic amount. In the case of using a platinum-based catalyst as the (D) component, the amount of platinum metal contained in the platinum-based catalyst is practically preferable for the hot-melt property of the present invention The amount in the curable silicone composition is in the range of 0.01 to 1000 ppm in terms of weight unit, and the amount in the range of 0.1 to 500 ppm is particularly preferred.

(E) Silicon dioxide As the (E) component silicon dioxide, for example, vapor-phase silicon dioxide, wet silicon dioxide, crystalline silicon dioxide, precipitating silicon dioxide, and the like can be cited. In addition, silicon dioxide can also be surfaced with organosilicon compounds such as organoalkoxysilane compounds, organochlorosilane compounds, organosilazane compounds, low molecular weight silicone compounds, or silane coupling agents, titanate coupling agents, etc. Hydrophobic treatment.

Based on the total mass of the composition of the present invention, the compounding amount of component (E) can be preferably 0.01% by mass or more, more preferably 0.1% by mass or more, most preferably 0.5% by mass or more, especially 1 An amount of at least mass% is contained in the hot-melt curable silicone composition of the present invention, and may preferably be 20% by mass or less, more preferably 15% by mass or less, and most preferably 10% by mass or less The amount is contained in the hot-melt curable silicone composition of the present invention.

The hot-melt curable silicone composition of the present invention may contain optional components within a range that does not impair the purpose of the present invention. Examples of such optional components include acetylene compounds; organophosphorus compounds; vinyl siloxane compounds; hydrosilylation reaction inhibitors; crushed quartz, titanium oxide, magnesium carbonate, zinc oxide, iron oxide, diatomaceous earth, etc. ( E) Inorganic fillers other than silica (also called "inorganic fillers"); inorganic fillers obtained by hydrophobic treatment of the surface of such inorganic fillers by organosilicon compounds; no silicon atom bonding Hydrogen atom and silicon atom bonded alkenyl organopolysiloxane; tackifier; heat-resistant agent; cold-resistant agent; thermal conductivity filler; flame retardant; thixotropic agent; phosphor; carbon black and other pigments and dyes, etc. Coloring ingredients, solvents, etc.

The hydrosilylation reaction inhibitor is a component for inhibiting the hydrosilylation reaction of the organosilicon composition. Specifically, for example, acetylenes such as 1-ethynyl-2-cyclohexanol, amines, carboxylates, Reaction inhibitors such as phosphites. The addition amount of the reaction inhibitor is usually 0.001 to 5 mass% of the entire organosilicon composition.

(E) Inorganic fillers other than silicon dioxide include, for example, hollow fillers, silsesquioxane, fumed titanium dioxide, magnesium oxide, zinc oxide, iron oxide, aluminum hydroxide, magnesium carbonate, calcium carbonate, and zinc carbonate. , Layered mica, diatomaceous earth, glass fiber and other inorganic fillers; use organoalkoxysilane compounds, organochlorosilane compounds, organosilazane compounds and low molecular weight siloxane compounds and other organosilicon compounds for these fillers Fillers etc. after surface hydrophobization treatment. In addition, silicone rubber powder, silicone resin powder, etc. can also be blended. However, the blending amount of the inorganic filler is specifically preferably 20% by mass or less of the organosilicon composition, and particularly preferably 10% by mass or less.

Examples of phosphors include oxide phosphors, oxynitride phosphors, nitride phosphors, sulfide phosphors, which are widely used in light emitting diodes (LED), Yellow, red, green, blue light-emitting phosphors composed of sulfur oxide-based phosphors, fluoride-based phosphors, etc., and mixtures of at least two of them. As oxide-based phosphors, yttrium, aluminum, and garnet-based YAG-based green-yellow light-emitting phosphors containing cerium ions; Light body, and silicate green-yellow light emitting phosphor containing cerium and europium ions. As the oxynitride-based phosphor, a SIALON-based red-green light-emitting phosphor of silicon, aluminum, oxygen, and nitrogen containing europium ions can be exemplified. As the nitride-based phosphor, a CASN-based red light-emitting phosphor containing europium ions, calcium, strontium, aluminum, silicon, and nitrogen can be exemplified. As the sulfide-based phosphor, a ZnS-based green light-emitting phosphor containing copper ions or aluminum ions can be exemplified. As the sulfur oxide-based phosphor, a Y ₂ O ₂ S-based red light-emitting phosphor containing europium ions can be exemplified. As the fluoride-based phosphor, KSF phosphor (K ₂ SiF ₆ : Mn ⁴⁺ ) or the like can be mentioned.

As the coloring component, organic or inorganic pigments and dyes may be used alone or in combination of two or more. When a phosphor is used, the blending amount may be 90% by mass or less of the organosilicon composition, preferably 80% by mass or less, and particularly preferably 70% by mass or less. In addition, from the viewpoint of preventing interference of light in the display and improving color contrast, black pigments may also be used. Examples of black pigments include iron oxide, aniline black, activated carbon, graphite, carbon nanotubes, and carbon black. The blending amount of the coloring component is specifically 30% by mass or less of the organosilicon composition, preferably 15% by mass or less, and particularly preferably 5% by mass or less.

The hot-melt curable organosilicon composition of the present invention can be prepared by mixing the components. The mixing method of each component can be a conventionally well-known method, There is no restriction|limiting in particular, Usually, a uniform mixture is formed by simple stirring. In addition, when a solid component such as an inorganic filler is contained as an optional component, it is more preferable to use a mixing device for mixing. Such a mixing device is not particularly limited, and a single-shaft or double-shaft continuous mixer, a two-roll mill, a Ross mixer, a Hobart mixer, a dental mixer, a planetary mixer, a kneading mixer, a Henschel mixer, etc. may be mentioned.

The hot-melt curable silicone composition of the present invention can exhibit excellent mechanical properties, especially strength and elongation, even when it is molded into a film or sheet shape. Therefore, the hot-melt curable organosilicon composition of the present invention has excellent processing performance and can form a sealant and a laminate film that can efficiently manufacture semiconductor packages and are used in the manufacture of semiconductor packages. Therefore, the hot-melt curable organosilicon composition of the present invention can be applied to the use of sheet or film sealants and lamination films when manufacturing semiconductor packages. [Sealant, film]

The present invention also relates to a sealing agent for semiconductors using the hot-melt curable organosilicon composition of the present invention. The shape of the sealant of the present invention is not particularly limited, but a film shape or a sheet shape is preferable. Therefore, the present invention also relates to a film obtained by curing the hot-melt curable organosilicon composition of the present invention. The film of the present invention can be preferably applied to a film-like sealant for sealing semiconductor elements and a film for lamination. The semiconductor sealed by the sealant or film of the present invention is not particularly limited, and examples thereof include semiconductors such as SiC and GaN, particularly optical semiconductors such as power semiconductors and light-emitting diodes.

Even if the sealant or film of the present invention is in the form of a film or sheet, it can exhibit excellent mechanical properties, particularly strength and elongation, and therefore has excellent handling performance and can efficiently manufacture semiconductor packages. [Optical Semiconductor Device]

The present invention also relates to an optical semiconductor device containing the sealant of the present invention. As the optical semiconductor element, a light emitting diode (LED), a semiconductor laser, a photodiode, a phototransistor, a solid-state imaging device, a light-emitting body and a photoreceptor for an optical coupler can be exemplified, and a light-emitting diode is particularly preferred. (LED).

The light emitting diode (LED) emits light from the top, bottom, left, and right of the optical semiconductor element. Therefore, the components constituting the light emitting diode (LED) are preferably not a material that absorbs light, but more preferably a light transmittance Materials with high or high reflectivity. Therefore, the substrate on which the optical semiconductor element is mounted is also preferably a material with high light transmittance or high reflectance. Examples of substrates on which such optical semiconductor elements are mounted include conductive metals such as silver, gold, and copper; non-conductive metals such as aluminum and nickel; thermoplastic resins mixed with white pigments such as PPA and LCP; epoxy resins and BT resins. , Polyimide resins and silicone resins and other thermosetting resins containing white pigments; and ceramics such as alumina and aluminum nitride.

The optical semiconductor element of the present invention includes the encapsulant of the present invention that has excellent processing performance and can efficiently manufacture semiconductor packages, and therefore has excellent reliability. [Example]

The hot-melt curable silicone composition of the present invention will be described in detail with the following examples and comparative examples. [Examples 1 to 22 and Comparative Examples 1 to 5]

The components are mixed according to the composition (parts by weight) shown in Tables 1 to 4 to prepare a hot-melt curable organosilicon composition. In addition, hereinafter, Me represents a methyl group, Vi represents a vinyl group, Ph represents a phenyl group, and Ep represents a 3-glycidoxypropyl group.

Component a-1: average unit formula (ViMeSiO _2/2 ) ₂₅ (Ph ₂ SiO _2/2 ) ₃₀ (PhSiO _3/2 ) ₄₅ shows the resinous alkenyl group-containing organopolysiloxane component a-2: average resinous unit formula _{(ViMe 2 SiO 1/2) 25 (} PhSiO 3/2) 75 shown alkenyl group-containing organopolysiloxane silicon alumoxane component a-3: general formula _{(ViMe 2 SiO 1/2) (PhMeSiO} 2 / ₂ ) ₂₀ (ViMe ₂ SiO _1/2 ) linear alkenyl-containing organopolysiloxane component a-4: general formula (ViMeSiO _2/2 ) ₄ cyclic alkenyl-containing organopolysiloxane Oxyane component a-5: _{the resinous alkenyl group-containing organopolysiloxane represented by the general formula (ViMe 2} SiO _1/2 ) ₃ (PhSiO _3/2 ) component b-1: average unit formula (HMe ₂ SiO _{1 /2} ) ₆₀ (PhSiO _3/2 ) Resin-like organohydrogen polysiloxane component b-2 shown by _{40 : General formula (HMe 2} SiO _1/2 ) (Ph ₂ SiO _2/2 ) (HMe ₂ SiO _{1 /2} ) linear organohydrogen polysiloxane component c-1: average unit formula (ViMe ₂ SiO _1/2 ) ₂₅ (PhSiO _3/2 ) _{75 (EpMeSiO 2/2} ) ₄₀ Component c-2: Structural formula (Me ₂ SiO _2/2 ) (ViMeSiO _2/2 ) (EpSiO _3/2 ) shows the additive component c-3: Average unit formula (EpMeSiO _2/2 ) ₄₈ (ViSiO _{3/ 2} ) ₂₁ (PhSiO _3/2 ) Additive component c-4 shown by _{31 : general formula (ViMe 2} SiO _1/2 ) (Me ₂ SiO _2/2 ) ₃ Si (OMe) ₃ additive component c- 5: Average unit formula (ViMe ₂ SiO _1/2 ) ₁₅ (Me ₂ SiO _2/2 ) ₃₅ (PhSiO _3/2 ) ₅₀ Additive component d: platinum with a platinum concentration of 4.0% by mass and 1,3- Divinyl-1,1,3,3-tetramethyldisiloxane complex component e: 1-ethynyl-2-cyclohexanol (platinum catalyst inhibitor) component f: fumed silica Component g: carbon black [evaluation]

Based on JIS K 6251, the tensile strength (MPa) and the elongation at break (%) of the cured products of the obtained hot-melt curable silicone compositions of Examples 1 to 22 and Comparative Examples 1 to 5 were measured. Specifically, the hot-melt curable organosilicon compositions of Examples 1-22 and Comparative Examples 1-5 were heat-aged at 120°C for 5-10 minutes to obtain hot-melt cured products. The melt elastic modulus of these hot-melt cured products at 100°C is measured by a viscoelastic meter (MCR302 manufactured by Anton Paar) and is 30 to 300 Pa. A test piece with a thickness of 180 μm and a dumbbell-shaped No. 3 shape was produced. Using this test piece, the tensile strength (MPa) and the elongation at break (%) were measured at a tensile speed of 500 mm/min. The results are shown in Tables 1 to 4. It can be said that a test piece with a tensile strength of 1 MPa or more and an elongation at break of 200% or more has excellent handling performance as a sealant film or laminate film.

[Table 1] [Table 1] ingredient Example 1 Example 2 Example 3 Example 4 Example 5 Example 6 Example 7 a-1 56.9 56.5 58.3 53.1 51.3 55.9 59.7 a-2 4 3.3 3.3 3.4 3.3 3.3 3.3 a-3 14.9 9.1 6.6 11.7 6.6 6.6 6.6 a-4 0.2 0.2 0.2 3.0 0.2 0.2 0.2 a-5 - 3.5 3.7 - 3.7 3.7 3.7 b-1 2.5 2.5 2.5 3.5 2.5 2.5 2.5 b-2 19.0 22.4 22.9 22.8 22.4 22.8 23.0 c-1 2.5 2.5 2.5 2.5 10.0 5.0 1.0 D 0.01 0.01 0.01 0.02 0.01 0.01 0.01 E 0.02 0.02 0.02 0.02 0.02 0.02 0.02 F 3 3 3 3 3 3 3 the sum of a ~ c components 100 100 100 100 100 100 100 Evaluation Tensile strength (MPa) 1.7 1.6 1.9 3.0 1.4 1.2 1.7 Elongation at break (%) 250 250 300 230 205 210 250

[Table 2] [Table 2] ingredient Example 8 Example 9 Example 10 Example 11 Example 12 Example 13 Example 14 Example 15 Example 16 a-1 58.0 58.2 47.1 47.1 47.1 58.0 53.1 58.2 58.2 a-2 3.3 3.3 - - - - - 3.3 3.3 a-3 6.6 6.6 25.3 25.3 25.3 15.9 25.1 6.6 6.6 a-4 0.2 0.2 2.3 2.3 2.3 1.2 - 0.2 0.2 a-5 3.7 3.7 - - - - - 3.7 3.7 b-1 2.5 2.5 4.2 4.2 4.2 3.0 1.6 1.0 2.0 b-2 23.2 23.0 18.6 18.6 18.6 19.4 17.7 24.5 23.5 c-1 - - 2.5 2.5 2.5 2.5 2.5 2.5 2.5 c-2 2.5 - - - - - - - - c-3 - 2.5 - - - - - - - D 0.01 0.01 0.02 0.02 0.02 0.01 0.01 0.01 0.01 E 0.02 0.02 0.02 0.02 0.02 0.02 0.02 0.02 0.02 F 3 3 3 3 3 3 3 3 3 G - - 0.1 0.3 2.0 - - - - the sum of a ~ c components 100 100 100 100 100 100 100 100 100 Evaluation Tensile strength (MPa) 1.1 1.2 2.5 2.6 2.9 2.1 2.0 1.1 1.3 Elongation at break (%) 280 270 250 260 220 230 270 400 450

[Table 3] [Table 3] ingredient Example 17 Example 18 Example 19 Example 20 Example 21 Example 22 a-1 60.1 59.6 55.4 59.6 55.8 51.0 a-2 3.3 3.3 3.3 3.3 3.3 3.3 a-3 6.6 6.6 6.6 6.6 6.6 6.6 a-4 0.2 0.2 0.2 0.2 0.2 0.2 a-5 3.7 3.7 3.7 3.7 3.7 3.7 b-1 2.5 2.5 2.5 2.5 2.5 2.5 b-2 23.1 23.1 23.3 23.1 22.9 22.7 c-1 - - - - - - c-2 0.5 1.0 5.0 - - - c-3 - - - 1.0 5.0 10.0 d 0.01 0.01 0.01 0.01 0.01 0.01 e 0.02 0.02 0.02 0.02 0.02 0.02 f 3 3 3 3 3 3 the sum of a ~ c components 100 100 100 100 100 100 Evaluation Tensile strength (MPa) 1.6 2.1 1.1 2.0 1.1 1.1 Elongation at break (%) 200 230 280 210 450 450

[Table 4] [Table 4] ingredient Comparative example 1 Comparative example 2 Comparative example 3 Comparative example 4 Comparative example 5 a-1 60.6 58.0 58.2 58.1 58.5 a-2 3.3 3.3 3.3 3.3 3.3 a-3 6.6 6.6 6.6 6.6 6.6 a-4 0.2 0.2 0.2 0.2 0.2 a-5 3.7 3.7 3.7 3.7 3.7 b-1 2.5 2.5 2.5 - 5.7 b-2 23.1 23.2 23.0 25.6 19.5 c-1 - - - 2.5 2.5 c-4 - 2.5 - - - c-5 - - 2.5 - - D 0.01 0.01 0.01 0.01 0.01 E 0.02 0.02 0.02 0.02 0.02 f 3 3 3 3 3 the sum of a ~ c components 100 100 100 100 100 Evaluation Tensile strength (MPa) 1.0 0.9 1.2 0.5 3.0 Elongation at break (%) 110 250 170 630 100 [Industrial availability]

The hot-melt curable organosilicon composition of the present invention can be formed into a film or sheet with excellent handling performance, so it can be applied to the use of sheet or film sealants and laminate films in the manufacture of semiconductor packages .

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Claims (12)

A solvent-free hot-melt curable organosilicon composition comprising: (A) Alkenyl-containing organopolysiloxane, which has at least two alkenyl groups in one molecule; (B) Resin-like organohydrogenpolysiloxane , Relative to the total mass of the composition, it is 0.1 ~ 5 mass%, and there are at least two silicon atoms bonded to hydrogen atoms in one molecule; (C) an additive represented by the following average unit formula (C-1): (R ¹ ₃ SiO _1/2 ) _a (R ¹ ₂ SiO _2/2 ) _b (R ¹ SiO _3/2 ) _{c In the} formula, R ¹ is the same or different containing alkyl, aryl, alkenyl, and aralkyl groups , Or epoxy organic group or alkoxy group, wherein at least one R ¹ is an alkenyl group, and at least one R ¹ is an epoxy-containing organic group, and a, b, and c are numbers satisfying the following conditions respectively : 0 ≤ a ≤ 1.0, 0 ≤ b ≤ 1.0, 0 ≤ c ＜ 0.9, and a + b + c = 1; (D) catalyst for hydrosilylation reaction; and (E) silicon dioxide. The hot-melt curable silicone composition according to claim 1, wherein the component (A) contains a _{resinous organopolysiloxane containing at least one (Ar 2} SiO _2/2 ) unit. The hot-melt curable silicone composition according to claim 1 or 2, wherein the component (B) is represented by the following (B-1) average unit formula: (R ³ ₃ SiO _1/2 ) _a (R ³ ₂ SiO _2/2 ) _b (R ³ SiO _3/2 ) _c (SiO _4/2 ) _d (XO _1/2 ) _{e In the} formula, R ³ is the same or different halogen substituted or unsubstituted monovalent hydrocarbon group , Where at least two R ³ are hydrogen atoms, X is a hydrogen atom or an alkyl group, a, b, c, d and e are numbers satisfying the following conditions: 0 ≤ a ≤ 1.0, 0 ≤ b ≤ 1.0, 0 ≤ c <0.9, 0 ≤ d <0.5, 0 ≤ e <0.4, a + b + c + d = 1.0, and c + d> 0. The hot-melt curable silicone composition according to claim 3, wherein, in the average unit formula (B-1), a is in the range of 0.1 ≤ a ≤ 0.9, and b is 0 ≤ b ≤ 0.8 The range, c is the range of 0.1 ≤ c ≤ 0.9, d is the range of 0 ≤ d ≤ 0.4, and e is the range of 0 ≤ e ≤ 0.3. The hot-melt curable silicone composition according to any one of claims 1 to 4, wherein, in the average unit formula (C-1), a is in the range of 0 ≤ a ≤ 0.9, and b is 0.1 ≤ b ≤ 0.9, and c is 0.01 ≤ c ≤ 0.8. The hot-melt curable silicone composition according to any one of claims 1 to 5, wherein the content of the alkenyl group contained in the component (C) is 5 mol% or more of the sum of ^{R 1.} The hot-melt curable silicone composition according to any one of claims 1 to 6, wherein the content of the epoxy group-containing organic group contained in the component (C) is 5 moles of the sum of ^{R 1} Ear% or more. The curable silicone composition according to any one of claims 1 to 7, which contains linear, resinous, and cyclic organopolysiloxanes as the (A) component. A film obtained by curing the hot-melt curable organosilicon composition according to any one of claims 1 to 8. A sealant composed of the hot-melt curable organosilicon composition according to any one of claims 1 to 8. An optical semiconductor element comprising the sealant according to claim 10. The optical semiconductor device according to claim 11, wherein the optical semiconductor is a light emitting diode.