KR20160031256A - Inorganic filler, epoxy resin composition comprising the same and light emitting element comprising isolation layer using the same - Google Patents

Abstract

The present invention relates to an inorganic filler, an epoxy resin composition comprising the same, and a light emitting device comprising an insulation layer using the epoxy resin composition. The inorganic filler according to one embodiment of the present invention comprises an agglomerate which is agglomerated inorganic particles in plate shapes, and forms ceramics including two or more elements selected from the group consisting of C, N, and O, in a pore inside the agglomerate. Therefore, the epoxy resin composition has good dispersibility, excellent insulation performance, and high heat conductivity.

Description

TECHNICAL FIELD [0001] The present invention relates to an inorganic filler, an epoxy resin composition containing the filler, and an insulating layer using the same. BACKGROUND ART [0002]

The present invention relates to an inorganic filler, and more particularly, to an inorganic filler contained in an epoxy resin composition.

BACKGROUND ART Light emitting devices including light emitting devices such as light emitting diodes (LEDs) are used as various light sources. With the development of semiconductor technology, high output of light emitting devices is accelerating. In order to stably cope with a large amount of light and heat emitted from such a light emitting element, heat radiation performance of the light emitting element is required.

In addition, as electronic components become more highly integrated and higher in capacity, there is a growing interest in heat dissipation of printed circuit boards on which electronic components are mounted.

Generally, an epoxy resin composition including an epoxy compound, a curing agent and an inorganic filler may be used for an insulating layer of a light emitting element or a printed circuit board.

At this time, the inorganic filler may include boron nitride. However, the plate-shaped boron nitride has an excellent thermal conductivity, but has an anisotropic heat conduction characteristic. In order to solve this problem, it is possible to use a agglomerate of plate-like boron nitride, but the heat conduction performance may be lowered due to the pores in the aggregate, and the binding force between the boron nitride of the plate is weak,

SUMMARY OF THE INVENTION The present invention provides an inorganic filler contained in an epoxy resin composition.

An inorganic filler according to an embodiment of the present invention includes a coagulated body in which plate-like inorganic particles are aggregated, and a ceramic containing at least two elements selected from the group consisting of C, N and O is formed in the pores in the aggregate.

The plate-like inorganic particles may include at least one of graphite and boron nitride (BN).

The ceramic may comprise silicon oxycarbonitride (SiCNO) or silicon carbonitride (SiCN).

The silicon oxycarbonitride or the silicon carbonitride may be formed from polysilazane (PSZ).

The ceramic may include at least one of aluminum oxide, silicon oxide and titanium oxide including an alkoxide group.

The alkoxide group may be selected from the group consisting of C ₁ to C ₆ alkyl.

The ceramic may be formed from at least one of aluminum alkoxide, silicon alkoxide, and titanium alkoxide.

An epoxy resin composition according to an embodiment of the present invention includes an epoxy compound and an aggregate in which plate-shaped inorganic particles are aggregated, and a ceramic containing at least two elements selected from the group consisting of C, N, and O in the pores in the aggregate And an inorganic filler to be formed.

Aggregates in which the boron nitride is aggregated with respect to the volume ratio of the epoxy compound 10 may be contained in a volume ratio of 10 to 60.

Aggregates in which boron nitride is agglomerated with respect to the volume ratio of the epoxy compound 10 may be contained in a volume ratio of 15 to 55.

Aggregates in which the boron nitride is aggregated with respect to the volume ratio of the epoxy compound 10 may be included in a volume ratio of 45 to 55.

The epoxy compound may include at least one selected from the group consisting of a crystalline epoxy compound, an amorphous epoxy compound, and a silicone epoxy compound.

A light emitting device module according to an embodiment of the present invention includes a substrate, an insulating layer formed on the substrate, a circuit pattern formed on the insulating layer, and a light emitting device formed on the insulating layer, An epoxy resin composition comprising an inorganic filler including an epoxy compound and an agglomerated plate-like inorganic particle aggregate, wherein a ceramic containing at least two elements selected from the group consisting of C, N and O is formed in the pores in the agglomerate, .

According to an embodiment of the present invention, an inorganic filler contained in an epoxy resin composition applied to a printed circuit board and a light emitting device module can be obtained. Thus, an epoxy resin composition having good dispersibility, excellent insulation performance, high thermal conductivity, and excellent adhesive strength and processability can be obtained. In particular, it is possible to obtain an inorganic filler having excellent heat conduction properties of isotropy.

Figures 1-2 illustrate a method of coating the surface of an inorganic filler in accordance with one embodiment of the present invention.
Figure 3 shows the morphology of the boron nitride aggregate before filling the void.
Figure 4 shows the shape of the aggregate of boron nitride after filling the voids.
5 is a cross-sectional view of a printed circuit board according to an embodiment of the present invention.
6 is a cross-sectional view of a light emitting device module according to an embodiment of the present invention.

The present invention is capable of various modifications and various embodiments, and specific embodiments are illustrated and described in the drawings. It should be understood, however, that the invention is not intended to be limited to the particular embodiments, but includes all modifications, equivalents, and alternatives falling within the spirit and scope of the invention.

The terms including ordinal, such as second, first, etc., may be used to describe various elements, but the elements are not limited to these terms. The terms are used only for the purpose of distinguishing one component from another. For example, without departing from the scope of the present invention, the second component may be referred to as a first component, and similarly, the first component may also be referred to as a second component. And / or < / RTI > includes any combination of a plurality of related listed items or any of a plurality of related listed items.

The terminology used in this application is used only to describe a specific embodiment and is not intended to limit the invention. The singular expressions include plural expressions unless the context clearly dictates otherwise. In the present application, the terms "comprises" or "having" and the like are used to specify that there is a feature, a number, a step, an operation, an element, a component or a combination thereof described in the specification, But do not preclude the presence or addition of one or more other features, integers, steps, operations, elements, components, or combinations thereof.

Unless defined otherwise, all terms used herein, including technical or scientific terms, have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. Terms such as those defined in commonly used dictionaries are to be interpreted as having a meaning consistent with the contextual meaning of the related art and are to be interpreted as either ideal or overly formal in the sense of the present application Do not.

Whenever a portion of a layer, film, region, plate, or the like is referred to as being "on" another portion, it includes not only the case where it is "directly on" another portion, but also the case where there is another portion in between. Conversely, when a part is "directly over" another part, it means that there is no other part in the middle.

Hereinafter, embodiments will be described in detail with reference to the accompanying drawings, wherein like or corresponding elements are denoted by the same reference numerals, and redundant description thereof will be omitted.

An epoxy resin composition according to an embodiment of the present invention includes an epoxy compound and an inorganic filler. More specifically, the epoxy resin composition according to one embodiment of the present invention comprises 3 to 40% by volume, preferably 3 to 20% by volume of an epoxy compound, 0.5 to 10% by volume, preferably 0.5 to 5% by volume of a curing agent, 95% by volume, more preferably 75% by volume to 95% by volume. When the epoxy compound, the curing agent and the inorganic filler are contained in these numerical ranges, an epoxy resin composition having good thermal conductivity, room temperature safety, and dispersibility can be obtained. Particularly, when the inorganic filler is contained in an amount exceeding 95 vol%, the content of the epoxy compound is relatively reduced, and the microporosity is formed between the inorganic filler and the epoxy compound, so that the thermal conductivity may be lowered. Also, even when the inorganic filler is contained in an amount of less than 50 vol%, the thermal conductivity may be lowered.

At this time, the inorganic filler includes aggregates in which plate-like inorganic particles are aggregated, and ceramics containing two or more elements selected from the group consisting of C, N and O may be formed in the pores in the aggregate.

At this time, the agglomerated plate-like inorganic particles may be contained in an amount of 10 to 60 volume parts, preferably 15 to 55 volume parts, more preferably 45 to 55 volume parts, based on 10 volume parts of the epoxy compound. When the epoxy compound and the aggregate satisfy these numerical ranges, an epoxy resin composition having both thermal conductivity and peel strength can be obtained. Particularly, if the aggregate is contained in an amount of less than 10 parts by volume based on 10 parts by volume of the epoxy compound, the thermal conductivity may be lowered. If the agglomerate is contained in an amount exceeding 60 volume ratio with respect to the volume ratio of the epoxy compound 10, the brittle of the epoxy resin composition may be increased and the peel strength may be lowered.

Here, the epoxy compound may include at least one of a crystalline epoxy compound, amorphous epoxy compound, and silicone epoxy compound.

The crystalline epoxy compound may include a mesogen structure. Mesogen is a liquid crystal  It is a basic unit and includes a rigid structure.

The amorphous epoxy compound may be a conventional amorphous epoxy compound having two or more epoxy groups in the molecule, for example, a glycidyl ether compound derived from bisphenol A or bisphenol F. The amorphous epoxy compound may contain 3 to 40 parts by volume of the amorphous epoxy compound relative to 10 parts by volume of the crystalline epoxy compound. When the crystalline epoxy compound and the amorphous epoxy compound are contained at such a ratio, stability at room temperature can be enhanced.

The silicone epoxy compound may be contained in a proportion of 3 to 40 parts by volume based on 10 parts by volume of the crystalline epoxy compound. When the crystalline epoxy compound and the silicon epoxy compound are contained in this ratio, thermal conductivity and heat resistance can be increased.

The curing agent contained in the epoxy resin composition according to one embodiment of the present invention is selected from the group consisting of an amine curing agent, a phenol curing agent, an acid anhydride curing agent, a polymercaptan curing agent, a polyaminoamide curing agent, an isocyanate curing agent and a block isocyanate And a curing agent, and two or more kinds of curing agents may be mixed and used.

The epoxy resin composition according to an embodiment of the present invention includes an aggregate in which plate-shaped inorganic particles are agglomerated, and a ceramic in which a ceramic containing at least two elements selected from the group consisting of C, N and O is formed in the pores in the aggregate And a filler.

As described above, when the inorganic filler includes agglomerates rolled up into plate-like inorganic particles, it is possible to have an isotropic heat conductive property uniform in heat conduction performance in all directions, and to improve the dispersibility and the insulation performance. Particularly, when the voids in the aggregated body are filled, the air layer in the aggregated body is minimized and the heat conduction performance can be enhanced, and the bonding force between the plate-shaped inorganic particles forming the aggregated body can be increased, and cracking of the aggregated body can be prevented.

Here, the plate-like inorganic particles may include at least one of graphite and boron nitride (BN). Alternatively, the plate-like inorganic particles may include a hybrid filler in which graphite and boron nitride are present in a plane, respectively.

Meanwhile, the ceramic filled in the pores in the agglomerate may include silicon oxycarbonitride (SiCNO) or silicon carbonitride (SiCN). At this time, SiCNO or SiCN can be formed from polysilazane (PSZ) of the formula (1).

[Chemical Formula 1]

Wherein R ¹ , R ² and R ³ can each be selected from the group consisting of H, C ₁ -C ₃ alkyl, C ₂ -C ₃ alkene, C ₂ -C ₃ alkyne, and n is a positive integer.

Alternatively, the ceramic filled in the voids in the agglomerate may include at least one of aluminum oxide including an alkoxide group, silicon oxide including an alkoxide group, and titanium oxide including an alkoxide group. Wherein the aluminum oxide is formed from a hydrolysis reaction and a dehydration condensation reaction of an aluminum alkoxide of formula (2), the silicon oxide is formed from a hydrolysis reaction and a dehydration condensation reaction of the silicon alkoxide of formula (3) 4 < / RTI > titanium alkoxide, and a dehydration condensation reaction.

(2)

Here, R ¹ to R ³ may be selected from the group consisting of H and C ₁ to C ₆ alkyl, respectively.

(3)

Here, R ¹ to R ⁴ may be selected from the group consisting of H and C ₁ to C ₆ alkyl, respectively.

[Chemical Formula 4]

Here, R ¹ to R ⁴ may be selected from the group consisting of H and C ₁ to C ₆ alkyl, respectively.

The mechanism for forming a silicon oxide containing an alkoxide group from a silicon alkoxide is shown in the following reaction formula.

Figs. 1 and 2 show a method of filling ceramics with voids of agglomerated aggregates of plate-like inorganic particles according to an embodiment of the present invention. For convenience of explanation, the plate-like inorganic particles are plate-like boron nitride, and the ceramic is SiCNO 3, but the present invention is not limited thereto.

Referring to FIGS. 1 and 2, the boron nitride aggregate 200 is mixed with polysilazane (S110). Figure 3 shows the morphology of the boron nitride aggregate 200. The EDX analysis of the surface of the boron nitride aggregate 200 of FIG. 3 reveals that B and N show a ratio of 75.33 wt% and 24.67 wt%, respectively. When the cross section is analyzed by EDX, B is 73.58 wt% and N is 26.42 wt% . For example, the polysilazane may be a monomer or an oligomer. After 30 g of polysilazane and 30 g of the boron nitride aggregate 200 are stirred for 5 minutes, a solvent, for example, For example, acetone can be used for washing.

For this purpose, the boron nitride aggregate 200 may be etched in advance using a hydrofluoric acid (HF) -based solution or the like. When the boron nitride aggregate 200 is etched, the reactivity with the polysilazane can be increased.

Accordingly, the liquid polysilazane can be filled in the voids and on the surface of the boron nitride aggregate 210.

Next, the liquid polysilazane in the pores and on the surface of the boron nitride aggregate 210 is polymerized (S110). For this purpose, the boron nitride aggregate 210 can be treated at 160 to 180 DEG C for 18 to 24 hours. Accordingly, the polysilazane monomer or oligomer may be crosslinked through a dehydration condensation reaction to cover the voids of the boron nitride aggregate 220 or be coated on the surface.

Then, the boron nitride aggregate 220 is sintered (S120). For this purpose, the boron nitride aggregate 220 can be pyrolysed at 700 to 800 ° C for 2 to 3 hours. Through the thermal decomposition process, CH ₄ , C ₂ H ₄ , C ₂ H ₆ , and NH ₃ of the polysilazane polymer are released, and the boron nitride aggregate 230 in which pores and surfaces are filled with SiCNO 3 ceramics can be obtained. Figure 4 shows the morphology of the boron nitride agglomerates with voids filled with SiCNO. EDX analysis of the surface of the aggregate of boron nitride in FIG. 4 shows that the ratio of B is 50.23 wt%, C is 9.00 wt%, N is 7.56 wt%, O is 4.69 wt%, Si is 28.53 wt% According to the analysis, B represents 53.40 wt%, C represents 9.16 wt%, N represents 12.14 wt%, O represents 5.93 wt%, and Si represents 19.38 wt%.

If the pyrolysis process in step S120 is performed in a nitrogen atmosphere, the pores may be filled with a ceramic containing SiCN.

When a liquid ceramic precursor such as polysilazane, aluminum alkoxide, silicon alkoxide, titanium alkoxide or the like is mixed with a boron nitride aggregate and then heated, the liquid ceramic precursor is impregnated into the pores of the boron nitride aggregate, So that it is easy to fill the voids.

The epoxy resin composition according to an embodiment of the present invention may further include at least one selected from the group consisting of aluminum oxide, aluminum nitride, magnesium oxide, and boron nitride.

An epoxy resin composition comprising an inorganic filler according to an embodiment of the present invention can be applied to a printed circuit board. 5 is a cross-sectional view of a printed circuit board according to an embodiment of the present invention.

Referring to FIG. 5, a printed circuit board 100 includes a substrate 110, an insulating layer 120, and a circuit pattern 130.

The substrate 110 may be made of copper, aluminum, nickel, gold, platinum, and alloys thereof.

On the substrate 110, an insulating layer 120 made of an epoxy resin composition including an inorganic filler according to an embodiment of the present invention is formed.

On the insulating layer 120, a circuit pattern 130 is formed. The circuit pattern 130 may be formed of a metal such as copper or nickel.

The insulating layer 120 insulates the metal plate 110 from the circuit pattern 130.

The epoxy resin composition containing the inorganic filler according to one embodiment of the present invention can also be applied to the light emitting device module. 6 is a cross-sectional view of a light emitting device module according to an embodiment of the present invention.

Referring to FIG. 6, the light emitting device module 400 includes a substrate 410, an insulating layer 420 formed on the substrate 410, a circuit pattern 430 formed on the insulating layer 420, And a light emitting device 430 formed on the substrate 420.

The substrate 410 may be made of copper, aluminum, nickel, gold, platinum, and alloys thereof.

The insulating layer 420 may include an epoxy resin composition comprising an inorganic filler according to one embodiment of the present invention.

Although not shown, a seed layer may be formed between the insulating layer 420 and the circuit pattern 430 to increase the adhesion between the insulating layer 420 and the circuit pattern 430.

Hereinafter, the present invention will be described more specifically with reference to examples and comparative examples.

≪ Example 1 >

3.75 vol% of 4,4'-biphenol ether diglycidyl ether, 1.875 vol% of amorphous epoxy compound of formula (5) and 1.875 vol% of silicon epoxy compound of formula (6), 4,4'-diamine 1.25 vol% of minodiphenylsulfone and 1.25 vol% of an acid anhydride-based curing agent of the formula (7) were mixed.

[Chemical Formula 5]

[Chemical Formula 6]

Wherein R ¹ to R ⁶ can each be selected from the group consisting of H, Cl, Br, F, C ₁ -C ₃ alkyl, C ₁ -C ₃ alkene, C ₁ -C ₃ alkyne, have. Here, R ¹ to R ⁶ may be a phenyl group.

(7)

Then, 26 vol% of alumina and 25 vol% of boron nitride filled with SiCNO 3 (where boron nitride filled with SiCNO 3 was mixed with polysilazane, which was a lump of plate-like boron nitride, was mixed with polysilazane, And an average density of 2.246 g / cm < ³ > and a porosity ratio of 1% or less) was added, and the mixture was stirred for 2 hours. The stirred solution was uniformly coated on a copper plate and then cured at 150 DEG C for 1 hour and 30 minutes at a constant pressure.

≪ Example 2 >

3.75 vol% of 4,4'-biphenol ether diglycidyl ether, 1.875 vol% of amorphous epoxy compound of formula (5) and 1.875 vol% of silicon epoxy compound of formula (6), 4,4'-diamine 1.25 vol% of minodiphenylsulfone and 1.25 vol% of an acid anhydride-based curing agent of the formula (7) were mixed.

Then, 35 vol% of alumina and boron nitride filled with SiCNO 3 as a pore (where boron nitride filled with SiCNO 3 is mixed with polysilazane, which is a lump of plate-like boron nitride, is mixed with polysilazane, and then heated at 180 ° C. for 24 hours Treated and pyrolyzed at 700 ° C for 2 hours, and the average density was 2.246 g / cm ³ and the porosity ratio was 1% or less), and the mixture was stirred for 2 hours. The stirred solution was uniformly coated on a copper plate and then cured at 150 DEG C for 1 hour and 30 minutes at a constant pressure.

≪ Example 3 >

3.75 vol% of 4,4'-biphenol ether diglycidyl ether, 1.875 vol% of amorphous epoxy compound of formula (5) and 1.875 vol% of silicon epoxy compound of formula (6), 4,4'-diamine 1.25 vol% of minodiphenylsulfone and 1.25 vol% of an acid anhydride-based curing agent of the formula (7) were mixed.

Then, 50 vol% of alumina and 50 vol% of boron nitride filled with SiCNO 3 (where boron nitride filled with SiCNO 3 is mixed with polysilazane, which is a lump of plate-like boron nitride, is mixed with polysilazane, , And pyrolysis was carried out at 700 ° C for 2 hours, the average density was 2.246 g / cm ³ and the porosity ratio was 1% or less), and the mixture was stirred for 2 hours. The stirred solution was uniformly coated on a copper plate and then cured at 150 DEG C for 1 hour and 30 minutes at a constant pressure.

<Example 4>

3.75 vol% of 4,4'-biphenol ether diglycidyl ether, 1.875 vol% of amorphous epoxy compound of formula (5) and 1.875 vol% of silicon epoxy compound of formula (6), 4,4'-diamine 1.25 vol% of minodiphenylsulfone and 1.25 vol% of an acid anhydride-based curing agent of the formula (7) were mixed.

Then, 58 vol% of alumina and 5 vol% of boron nitride filled with SiCNO 3 (where boron nitride filled with SiCNO 3 as a pore is a mixture of boron nitride aggregates, which is a lump of plate-like boron nitride, is mixed with polysilazane, , And pyrolysis was performed at 700 ° C for 2 hours, and the average density was 2.246 g / cm ³ and the porosity ratio was 1% or less), and the mixture was stirred for 2 hours. The stirred solution was uniformly coated on a copper plate and then cured at 150 DEG C for 1 hour and 30 minutes at a constant pressure.

&Lt; Example 5 >

3.75 vol% of 4,4'-biphenol ether diglycidyl ether, 1.875 vol% of amorphous epoxy compound of formula (5) and 1.875 vol% of silicon epoxy compound of formula (6), 4,4'-diamine 1.25 vol% of minodiphenylsulfone and 1.25 vol% of an acid anhydride-based curing agent of the formula (7) were mixed.

Then, 66 vol% of alumina and boron nitride filled with SiCNO 3 as a pore (where boron nitride filled with SiCNO 3 is mixed with polysilazane, which is a lump of plate-like boron nitride, is mixed with polysilazane and then heated at 180 ° C. for 24 hours , And pyrolysis was performed at 700 ° C for 2 hours, and the average density was 2.246 g / cm ³ and the porosity ratio was 1% or less), and the mixture was stirred for 2 hours. The stirred solution was uniformly coated on a copper plate and then cured at 150 DEG C for 1 hour and 30 minutes at a constant pressure.

&Lt; Example 6 >

3.75 vol% of 4,4'-biphenol ether diglycidyl ether, 1.875 vol% of amorphous epoxy compound of formula (5) and 1.875 vol% of silicon epoxy compound of formula (6), 4,4'-diamine 1.25 vol% of minodiphenylsulfone and 1.25 vol% of an acid anhydride-based curing agent of the formula (7) were mixed.

Then, 75 vol% of alumina and boron nitride filled with SiCNO 3 with voids (wherein boron nitride filled with SiCNO 3 was mixed with polysilazane, which was a lump of plate-like boron nitride, was mixed with polysilazane, And the pyrolysis was carried out at 700 ° C for 2 hours, and the average density was 2.246 g / cm ³ and the porosity ratio was 1% or less), and the mixture was stirred for 2 hours. The stirred solution was uniformly coated on a copper plate and then cured at 150 DEG C for 1 hour and 30 minutes at a constant pressure.

&Lt; Example 7 >

3.75 vol% of 4,4'-biphenol ether diglycidyl ether, 1.875 vol% of amorphous epoxy compound of formula (5) and 1.875 vol% of silicon epoxy compound of formula (6), 4,4'-diamine 1.25 vol% of minodiphenylsulfone and 1.25 vol% of an acid anhydride-based curing agent of the formula (7) were mixed.

Then, 82 vol% of alumina and boron nitride filled with SiCNO 3 as pores (where boron nitride filled with SiCNO 3 is mixed with polysilazane, which is a lump of plate-like boron nitride, is mixed with polysilazane, and then heated at 180 ° C. for 24 hours And an average density of 2.246 g / cm &lt; ³ &gt; and a porosity ratio of 1% or less) was added, and the mixture was stirred for 2 hours. The stirred solution was uniformly coated on a copper plate and then cured at 150 DEG C for 1 hour and 30 minutes at a constant pressure.

&Lt; Comparative Example 1 &

3.75 vol% of 4,4'-biphenol ether diglycidyl ether, 1.875 vol% of amorphous epoxy compound of formula (5) and 1.875 vol% of silicon epoxy compound of formula (6), 4,4'-diamine 1.25 vol% of minodiphenylsulfone and 1.25 vol% of an acid anhydride-based curing agent of the formula (7) were mixed.

Then, 26vol% of alumina and boron nitride was added (here, boron nitride is a lump of boron nitride agglomerates of agglomerated boron nitride plate-shaped, and the average density was 2.075g / cm ^3, the void ratio being 8%) 64vol%, and Stir 2 h. The stirred solution was uniformly coated on a copper plate and then cured at 150 DEG C for 1 hour and 30 minutes at a constant pressure.

&Lt; Comparative Example 2 &

3.75 vol% of 4,4'-biphenol ether diglycidyl ether, 1.875 vol% of amorphous epoxy compound of formula (5) and 1.875 vol% of silicon epoxy compound of formula (6), 4,4'-diamine 1.25 vol% of minodiphenylsulfone and 1.25 vol% of an acid anhydride-based curing agent of the formula (7) were mixed.

Then, 35vol% of alumina and boron nitride was added (here, boron nitride is a lump of boron nitride agglomerates of agglomerated boron nitride plate-shaped, and the average density was 2.075g / cm ^3, the void ratio being 8%) 55vol%, and Stir 2 h. The stirred solution was uniformly coated on a copper plate and then cured at 150 DEG C for 1 hour and 30 minutes at a constant pressure.

&Lt; Comparative Example 3 &

3.75 vol% of 4,4'-biphenol ether diglycidyl ether, 1.875 vol% of amorphous epoxy compound of formula (5) and 1.875 vol% of silicon epoxy compound of formula (6), 4,4'-diamine 1.25 vol% of minodiphenylsulfone and 1.25 vol% of an acid anhydride-based curing agent of the formula (7) were mixed.

Then, 50vol% of alumina and boron nitride was added (here, boron nitride is a lump of boron nitride agglomerates of agglomerated boron nitride plate-shaped, and the average density was 2.075g / cm ^3, the void ratio being 8%) 40vol%, and Stir 2 h. The stirred solution was uniformly coated on a copper plate and then cured at 150 DEG C for 1 hour and 30 minutes at a constant pressure.

&Lt; Comparative Example 4 &

3.75 vol% of 4,4'-biphenol ether diglycidyl ether, 1.875 vol% of amorphous epoxy compound of formula (5) and 1.875 vol% of silicon epoxy compound of formula (6), 4,4'-diamine 1.25 vol% of minodiphenylsulfone and 1.25 vol% of an acid anhydride-based curing agent of the formula (7) were mixed.

Then, 58vol% of alumina and boron nitride was added (here, boron nitride is a lump of boron nitride agglomerates of agglomerated boron nitride plate-shaped, and the average density was 2.075g / cm ^3, the void ratio being 8%) 32vol%, and Stir 2 h. The stirred solution was uniformly coated on a copper plate and then cured at 150 DEG C for 1 hour and 30 minutes at a constant pressure.

&Lt; Comparative Example 5 &

3.75 vol% of 4,4'-biphenol ether diglycidyl ether, 1.875 vol% of amorphous epoxy compound of formula (5) and 1.875 vol% of silicon epoxy compound of formula (6), 4,4'-diamine 1.25 vol% of minodiphenylsulfone and 1.25 vol% of an acid anhydride-based curing agent of the formula (7) were mixed.

Then, 66vol% of alumina and boron nitride was added (here, boron nitride is a lump of boron nitride agglomerates of agglomerated boron nitride plate-shaped, and the average density was 2.075g / cm ^3, the void ratio being 8%) 24vol%, and Stir 2 h. The stirred solution was uniformly coated on a copper plate and then cured at 150 DEG C for 1 hour and 30 minutes at a constant pressure.

&Lt; Comparative Example 6 >

3.75 vol% of 4,4'-biphenol ether diglycidyl ether, 1.875 vol% of amorphous epoxy compound of formula (5) and 1.875 vol% of silicon epoxy compound of formula (6), 4,4'-diamine 1.25 vol% of minodiphenylsulfone and 1.25 vol% of an acid anhydride-based curing agent of the formula (7) were mixed.

Then, 74vol% of alumina and boron nitride was added (here, boron nitride is a lump of boron nitride agglomerates of agglomerated boron nitride plate-shaped, and the average density was 2.075g / cm ^3, the void ratio being 8%) 16vol%, and Stir 2 h. The stirred solution was uniformly coated on a copper plate and then cured at 150 DEG C for 1 hour and 30 minutes at a constant pressure.

&Lt; Comparative Example 7 &

3.75 vol% of 4,4'-biphenol ether diglycidyl ether, 1.875 vol% of amorphous epoxy compound of formula (5) and 1.875 vol% of silicon epoxy compound of formula (6), 4,4'-diamine 1.25 vol% of minodiphenylsulfone and 1.25 vol% of an acid anhydride-based curing agent of the formula (7) were mixed.

Then, 82vol% of alumina and boron nitride was added (here, boron nitride is a lump of boron nitride agglomerates of agglomerated boron nitride plate-shaped, and the average density was 2.075g / cm ^3, the void ratio being 8%) 8vol%, and Stir 2 h. The stirred solution was uniformly coated on a copper plate and then cured at 150 DEG C for 1 hour and 30 minutes at a constant pressure.

<Experimental Example>

After curing the epoxy resin compositions obtained in Examples 1 to 7 and Comparative Examples 1 to 7, thermal conductivity was measured by an unsteady hot wire method using an LFA447 type thermal conductivity meter manufactured by NETZSCH. For this purpose, the epoxy resin composition was fabricated into a circular shape with a diameter of 0.5 inch, the laser pulse of 247 volts was injected into the upper part of the epoxy resin composition, and the time of equilibrium was measured to calculate the thermal conductivity. Then, the epoxy resin composition obtained in Examples 1 to 7 and Comparative Examples 1 to 7 was cured, and then a copper layer having a thickness of 62.5 mm was adhered, and the copper layer was lifted at a rate of 50 mm / min in a vertical direction And the peel strength was measured using a WI-M Tech equipment.

Table 1 shows the results.

Experiment number Thermal conductivity (W / mK) Peel strength (Kgf / cm) Example 1 14.1 0.30 Comparative Example 1 13.4 0.28 Example 2 16.9 0.38 Comparative Example 2 16.8 0.31 Example 3 21.76 0.67 Comparative Example 3 20.1 0.5 Example 4 19.4 0.70 Comparative Example 4 17.7 0.54 Example 5 18 0.75 Comparative Example 5 16.53 0.60 Example 6 16.1 0.81 Comparative Example 6 13.8 0.65 Example 7 12.7 0.9 Comparative Example 7 10.85 0.74

Referring to Table 1, the epoxy resin composition of Example 1, in which boron nitride aggregates filled with SiCNO 3 as a filler, was used as an inorganic filler, and the epoxy resin composition of Comparative Example 1 containing boron nitride agglomerates not filled with voids as an inorganic filler The heat conductivity is high and the peel strength is high.

Likewise, the epoxy resin compositions of Examples 2 to 7, in which boron nitride aggregates filled with SiCNO 3 as voids were filled as an inorganic filler, were prepared in the same manner as in Examples 2 to 7, except that the boron nitride agglomerates not filled with voids were used as inorganic fillers, 7, the thermal conductivity is high and the peel strength is high.

Particularly, Examples 3 to 7, in which the boron nitride agglomerates filled with SiCNO 3 in an amount of 10 to 60 parts by volume based on the volume ratio of the epoxy compound, were contained in an amount of 10 to 60 parts by volume, the thermal conductivity was improved by 8% Able to know. Further, according to Example 3, in which the boron nitride aggregate filled with SiCNO 3 in an amount of 45 to 55 parts by volume based on the volume ratio of the epoxy compound 10 was contained, an epoxy resin composition having a thermal conductivity of 21 W / mK or more and a peel strength of 0.6 Kgf / Can be obtained.

It will be apparent to those skilled in the art that various modifications and variations can be made in the present invention without departing from the spirit or scope of the present invention as defined by the following claims It can be understood that

100: printed circuit board
110: substrate
120: insulating layer
130: Circuit pattern

Claims (18)

Wherein an inorganic filler is provided, wherein the inorganic filler comprises platelike aggregates in which inorganic particles are plated, and a ceramic containing at least two elements selected from the group consisting of C, N and O is formed in the pores in the aggregate. The method according to claim 1,
Wherein the plate-like inorganic particles comprise at least one of graphite and boron nitride (BN). The method according to claim 1,
Wherein the ceramic comprises silicon oxycarbonitride (SiCNO) or silicon carbonitride (SiCN). The method of claim 3,
Wherein the silicon oxycarbonitride or the silicon carbonitride is formed from polysilazane (PSZ). The method according to claim 1,
Wherein the ceramic comprises at least one of aluminum oxide, silicon oxide and titanium oxide comprising an alkoxide group. 6. The method of claim 5,
Wherein said alkoxide group is selected from the group consisting of C ₁ to C ₆ alkyl. 6. The method of claim 5,
Wherein the ceramic is formed from at least one of aluminum alkoxide, silicon alkoxide, and titanium alkoxide. Epoxy compounds, and
An inorganic filler in which ceramic particles including at least two elements selected from the group consisting of C, N and O are formed in the pores in the aggregate,
&Lt; / RTI &gt; 9. The method of claim 8,
Wherein the plate-like inorganic particles comprise at least one of graphite and boron nitride (BN), and the ceramic comprises silicon oxycarbonitride (SiCNO). 9. The method of claim 8,
Wherein the plate-like inorganic particle comprises at least one of graphite and boron nitride (BN), and the ceramic comprises at least one of aluminum oxide, silicon oxide and titanium oxide containing an alkoxide group. 9. The method of claim 8,
Wherein the agglomerate of boron nitride is 10 to 60 parts by volume based on 10 parts by volume of the epoxy compound. 12. The method of claim 11,
Wherein the agglomerate of boron nitride is contained in an amount of 15 to 55 parts by volume relative to 10 parts by volume of the epoxy compound. 13. The method of claim 12,
Wherein an aggregate of boron nitride is dispersed in an amount of 45 to 55 parts by volume relative to 10 parts by volume of the epoxy compound. 9. The method of claim 8,
Wherein the epoxy compound comprises at least one selected from the group consisting of a crystalline epoxy compound, an amorphous epoxy compound, and a silicone epoxy compound. Board,
An insulating layer formed on the substrate,
A circuit pattern formed on the insulating layer, and
And a light emitting element formed on the insulating layer,
Wherein the insulating layer comprises an epoxy compound and an aggregate in which plate-shaped inorganic particles are aggregated, and an epoxy resin containing an inorganic filler in which a ceramic containing at least two elements selected from the group consisting of C, N and O is formed in the pores in the aggregate A light emitting device module comprising a resin composition. 16. The method of claim 15,
Wherein the ceramic comprises silicon oxycarbonitride (SiCNO) or silicon carbonitride (SiCN). 16. The method of claim 15,
Wherein the ceramic comprises at least one of aluminum oxide, silicon oxide, and titanium oxide including an alkoxide group. 16. The method of claim 15,
Wherein the aggregate is contained in a volume ratio of 10 to 60 with respect to the volume ratio of the epoxy compound.

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