JPH115907A - Highly heat-conductive resin composition having excellent water resistance - Google Patents

Abstract

PROBLEM TO BE SOLVED: To obtain a resin composition that has excellent thermal conductivity and water resistance and suffers little from bleeding of its ionic component even under high-temperature and high-humidity conditions, by treating an aluminum nitride powder with a phosphoric acid compound to give a water-resistant aluminum nitride powder, adding a flow improver to this powder, and blending a resin with this mixture. SOLUTION: This composition contains 100 pts.wt. resin, 50-600 pts.wt. water- resistant aluminum nitride powder comprising an aluminum nitride powder having a phosphoric acid compound incorporated therein, and a flow improver. Examples of the resin used include an epoxy resin, a silicone resin, a polyimide resin, and a polyester resin. The water-resistant aluminum nitride powder to be blended with the resin is obtained by treating an aluminum nitride powder with a phosphoric acid compound in the presence of water, adding a dispersant (e.g. an organic solvent) thereto, and blending this mixture and a flow improver comprising an inorganic powder having a lipophilic group on the surface (e.g. silica coated with a silicone).

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

TECHNICAL FIELD The present invention relates to a resin composition having excellent water resistance and thermal conductivity.

[0002]

2. Description of the Related Art Semiconductor devices such as semiconductor devices and ICs are protected from the outside by a package. As the degree of integration of semiconductor elements increases, the amount of heat generated from circuits using semiconductor elements also increases. It is an important technical problem to efficiently dissipate and remove the generated heat to the outside. Ceramics such as alumina having excellent heat radiation properties have been used for semiconductor packages, but in recent years, inexpensive polymer materials have been widely used because of their high cost.

[0003] However, since the polymer material itself has an extremely low thermal conductivity, the polymer material is actually added with an inorganic material having heat conductivity as a filler to improve the heat conductivity. I have.

The heat dissipation of a polymer material to which a thermally conductive inorganic material is added is determined by the thermal conductivity and the amount of the inorganic material added. In particular, the heat conductivity of the polymer material is greatly affected by the thermal conductivity of the inorganic material. At present, silica, alumina, boron nitride, and the like are used, but the use of aluminum nitride having higher thermal conductivity than these inorganic materials is shifting.

[0005] Aluminum nitride is hydrolyzed by moisture in the air to produce aluminum hydroxide and ammonia, which impairs the inherent thermal conductivity. Therefore, the surface of the aluminum nitride is treated with a phosphate compound to hydrolyze the aluminum nitride. A method for suppressing decomposition (hereinafter referred to as water resistance) has been disclosed (Japanese Patent Application No. 8-286780). Although aluminum nitride surface-treated by this method has high water resistance, it contains a large amount of leaching ionic components, so that it is difficult to use it as a resin filler such as a sealing material under high temperature and high humidity.
As described above, it is required that aluminum nitride used as a filler for resin has excellent water resistance and further contains a small amount of leaching ionic components.

[0006] Further, when treated with a phosphoric acid compound, the surface condition changes and the fluidity is significantly reduced as compared with the untreated one. Therefore, at the time of kneading with the resin, it is difficult for aluminum nitride to form an aggregate and to be uniformly dispersed in the resin. For example, therefore, when kneading aluminum nitride with a resin, it is necessary to knead the aluminum nitride while classifying it with a sieve, thereby increasing the number of steps and increasing the cost.

[0007]

SUMMARY OF THE INVENTION The present invention improves the fluidity of a water-resistant aluminum nitride powder, can be uniformly dispersed in a resin without forming aggregates, and has excellent thermal conductivity and water resistance. It is another object of the present invention to provide a resin composition which has a water-soluble property and less dissolves ionic components even under high temperature and high humidity.

[0008]

Means for Solving the Problems As a result of intensive studies, the present inventors treated aluminum nitride powder with a phosphoric acid compound, and added a specific fluidity improver to form an aggregate when kneading with a resin. Was found to be uniformly dispersed in the resin without forming the resin composition, and a resin composition having excellent thermal conductivity and water resistance was obtained, thereby completing the present invention.

That is, the present invention provides an excellent water-resistant composition comprising 50 to 600 parts by weight of a water-resistant aluminum nitride powder containing a phosphate compound in an aluminum nitride powder and a fluidity improver, based on 100 parts by weight of a resin. The present invention relates to a highly heat conductive resin composition having a property.

[0010]

DESCRIPTION OF THE PREFERRED EMBODIMENTS The present invention will be described below in detail.
Examples of the resin used in the present invention include epoxy resin, silicone resin, silicone rubber, polyimide resin, polycarbonate resin, polyamide resin, polyphenylene oxide resin, urethane resin, phenol resin, polyester resin, and fluorine resin.

The aluminum nitride powder used in the present invention may be any commercially available aluminum nitride powder. However, usually, the following production method is used. For example, there are a gas phase method in which an organic aluminum compound and ammonia are reacted and heated, an alumina reduction method in which a mixture of alumina and carbon is heated in nitrogen, and a direct nitriding method in which aluminum and nitrogen are reacted with each other. Manufactured products can also be used in the present invention. Among these, aluminum nitride powder produced by a gas phase method in which an organic aluminum compound is reacted with ammonia and heated, has good miscibility with the resin, can be added in a large amount to the resin, and has a high thermal conductivity. It is particularly preferable because a product can be obtained.

Treating the aluminum nitride powder of the present invention with a phosphate compound is an operation of bringing the aluminum nitride powder into contact with the phosphate compound to impart water resistance to the aluminum nitride powder. Examples of the operation method include a method in which aluminum nitride powder is dispersed in a phosphoric acid compound solution, a method in which the phosphoric acid compound solution is dusted on aluminum nitride powder and kneaded to form a paste.

When the aluminum nitride powder is treated with a phosphoric acid compound in the presence of water, the surface of the aluminum nitride is forcibly hydrolyzed to increase the amount of aluminum hydroxide, which is an active site reacting with the phosphorus compound. . This promotes the reaction with the phosphoric acid compound, resulting in high water resistance. This has been confirmed experimentally.
In addition, since this reaction is very fast, a water-resistant layer is immediately formed, and the characteristics of the aluminum nitride powder are not lost.

In the present invention, the phosphoric acid compound (aluminum phosphate) existing on the surface of the aluminum nitride powder has a P _{2 value.}
By identifying the content in O ₅ in terms, it is possible to impart excellent water resistance to the aluminum nitride powder.

Water resistant aluminum nitride treated with a phosphate compound
The phosphorous compound is converted to P₂O ₅0.1-1 in conversion
It is preferably contained in the range of 0% by weight, more preferably
Is from 0.3 to 8% by weight, most preferably from 0.5 to 6 weight%.
A range of% by weight is preferred. Water resistant aluminum nitride powder
P₂O₅If the content is less than 0.1% by weight, the desired water resistance
Properties cannot be obtained, and if it exceeds 10% by weight,
The desired water resistance and fluidity are obtained, but aluminum nitride
Oxygen content of aluminum nitride powder
This is not preferred because the thermal conductivity, which is the property of the polymer, is impaired. Also, not yet
Since phosphate compounds in the reaction increase, phosphate compounds that can be eluted
Increases, leading to an increase in eluting ionic components.
Not preferred.

The phosphoric acid compound referred to in the present invention reacts with aluminum in aluminum nitride powder to form an aluminum phosphate bond (Al-OP bond), and finally coats the aluminum nitride with a layer of aluminum phosphate. It means a phosphoric acid compound having the ability, for example, an inorganic phosphoric acid compound such as orthophosphoric acid, metaphosphoric acid, pyrophosphoric acid, polyphosphoric acid, phosphonic acid, methyl acid phosphate, ethyl acid phosphate, butyl acid phosphate, 2-ethylhexyl acid phosphate, lauryl Acid phosphates such as acid phosphate, palmityl acid phosphate, stearyl acid phosphate, oleyl acid phosphate, phenyl acid phosphate and nonylphenyl acid phosphate;
Examples thereof include mono- or dialkyl, alkenyl or aryl esters of pyrophosphoric acid or polyphosphoric acid such as ethylhexyl pyrophosphate, phosphonic acids such as methylenephosphonic acid and aminomethylenephosphonic acid, and organic phosphoric compounds such as esters thereof. Also, a mixture of two or more phosphoric acid compounds may be used.

The aluminum nitride powder used in the resin composition of the present invention can provide more excellent water resistance, can suppress the elution of ionic components, and can provide excellent fluidity (improvement in dispersibility in resin). Aluminum nitride powder. That is, it is an aluminum nitride powder containing a fluidity improver and containing a phosphoric acid compound in the aluminum nitride powder.

The aluminum nitride powder used in the resin composition of the present invention can be obtained by treating the aluminum nitride powder with a phosphate compound and further mixing a fluidity improver. The object of the present invention can be achieved by obtaining a resin composition using

The water-resistant aluminum nitride powder used in the present invention can be obtained by the production method disclosed in Japanese Patent Application No. 9-133111. The mixing of the fluidity improver can be carried out even after the phosphate compound treatment. It may be performed at the time of processing,
The mixing method of the fluidity improver is not limited as long as the fluidity improver can be uniformly mixed with the aluminum nitride powder.

The fluidity improver referred to in the present invention includes silica, alumina, titania, boron nitride, and inorganic powder having a lipophilic group on the surface. Further, a mixture of two or more fluidity improvers may be used. The particle size of these fluidity improvers is preferably 1 μm or less.

The inorganic powder having a lipophilic group on the surface of the present invention refers to an inorganic powder whose surface is covered with a resin, silicone, silicone oil, a fluorine compound or the like, and the surface of the inorganic powder is covered with a lipophilic group. Means inorganic powder. For example,
Silica having a lipophilic group on its surface (hereinafter referred to as water-repellent silica) and the like can be mentioned.

In particular, when an inorganic powder having a lipophilic group on the surface is used as the fluidity improver, the fluidity of the aluminum nitride powder is remarkably improved. By mixing
The water resistance is remarkably improved, and the compatibility with the resin is improved as compared with the others, so that the dispersibility in the resin is also significantly improved.

Further, when the inorganic powder having a lipophilic group on the surface is mixed by a method using an organic solvent as a dispersant, the water resistance is improved and the elution of ionic components is suppressed as compared with other methods. The effect is very large. By using the aluminum nitride powder obtained by such a method, it is possible to obtain a more reliable resin composition without deterioration even when used under high temperature and high humidity. The same effect can be obtained by containing any lipophilic coating agent on the surface of the inorganic powder. In particular, an inorganic powder in which the surface of the inorganic powder is coated with silicone oil is useful. The organic solvent as a dispersant used here may be anything as long as it is water-soluble,
Examples include methanol, ethanol, isopropanol, butanol, tetrahydrofuran (THF) and the like. Also, heptane, hexane, benzene, toluene,
A water-insoluble organic solvent such as chloroform may be used in combination.

In the water-resistant aluminum nitride powder used in the present invention, the flow improver is preferably added in an amount of 0.1 to 10% by weight, more preferably 0.5 to 10% by weight, based on the aluminum nitride powder. A range of 10% by weight is preferred. If the amount of the fluidity improver is less than 0.1% by weight, it is not preferable because an aluminum nitride powder having a desired fluidity cannot be obtained. Further, even if the addition amount exceeds 10% by weight, the effect of the fluidity improver is not changed, which is not preferable.

As the method of mixing the fluidity improver after the treatment with the phosphate compound, there are a method of mixing powders using a Henschel mixer, a V blender or the like, and a method of pulverizing and mixing using a ball mill. The latter method has a greater effect of improving performance.

As a method of mixing the fluidity improver during the treatment with the phosphate compound, a method in which aluminum nitride powder is dispersed in a phosphate compound solution and the fluidity improver is dispersed in a slurry, and a method in which the aluminum nitride powder is dispersed in the phosphate compound solution There are a method of kneading the fluidity improver into a kneading paste, a method of dispersing the fluidity improver in a phosphate compound solution in advance, and then treating the aluminum nitride powder with a phosphate compound. Also, the fluidity improver may be mixed in a slurry or paste form with a solvent.

The mixing of the inorganic powder having a lipophilic group on the surface with the use of a dispersant may be carried out at any time after the treatment with the phosphate compound or at the time of the treatment with the phosphate compound, and may be carried out at any time as long as uniform mixing is possible.

As a method of mixing after the phosphoric acid compound treatment, a water-resistant aluminum nitride powder or an inorganic powder having a lipophilic group on its surface is slurried and uniformly mixed using a mixer or a ball mill.

As a method of mixing at the time of the treatment with the phosphoric acid compound, a method in which an inorganic powder having a lipophilic group on the surface is previously made into a slurry or paste with a dispersant, and a method in which the phosphoric acid compound solution containing the dispersant is mixed There is a method in which an inorganic powder having a lipophilic group is directly added to the inner surface and mixed.
In the former case, the amount of the dispersant used may be small, and it can be produced at low cost. In particular, when the aluminum nitride powder is treated with an aqueous solution of an inorganic phosphoric acid such as orthophosphoric acid, and an inorganic powder having a lipophilic group on its surface is used as a fluidity improver, the mixture is fluidized using an organic solvent as a dispersant for uniform mixing. It is necessary to make the property improver into a slurry or paste.

The slurry of the aluminum nitride powder which has been treated with the phosphate compound and mixed with the fluidity improver is filtered,
After washing with water or an organic solvent in order to remove the excess phosphoric acid compound, it is dried and pulverized. By repeating this filtration to drying, an aluminum nitride powder having higher purity and excellent fluidity and water resistance and low elution of ionic components can be obtained. Further, any method may be used, such as a method of drying the water-resistant aluminum nitride powder treated with the phosphate compound as it is by spray drying, or a method of filtering and drying the cake as described above.

For filtering the aluminum nitride slurry, a Nutsche, centrifugal filter or the like is used. Further, the drying may be performed without filtering. When aluminum nitride powder is processed into a paste using a predetermined amount of a phosphoric acid compound and a fluidity improver, it is dried and ground as it is to obtain desired fluidity and water resistance, and ionic components are obtained. Water-resistant aluminum nitride powder having low dissolution property.

As a drying method, the filtered cake, slurry or paste is dried at 80 to 300 ° C. for 3 to 24 hours. A hot air dryer, a steam dryer, or the like is used as a dryer. For the pulverization, a jet mill, a sample mill, a ball mill or the like is used. Further, the pulverization referred to here is to convert the secondary particles into primary particles, and does not destroy the coating surface.

With respect to the water-resistant aluminum nitride powder having excellent fluidity and water resistance and low elution of ionic components obtained by the above method, the elution of ionic components is further suppressed by the following method. Can be. In other words, as a method for suppressing the elution of the ionic component, the aluminum phosphate bond (Al-O
-A method for promoting the production of P) and a method for removing leaching ionic components by washing. Further, the elution of the ionic component can be effectively suppressed by combining the heat treatment and the washing. By using the method for suppressing the elution of the ionic component, a water-resistant aluminum nitride powder having higher purity and excellent fluidity and water resistance and lower elution of the ionic component can be obtained.

By kneading the water-resistant aluminum nitride powder obtained by the above method and the resin, the water-resistant aluminum nitride powder has excellent thermal conductivity in which the water-resistant aluminum nitride powder is uniformly dispersed in the resin and deteriorates even under high temperature and high humidity. And a highly reliable resin composition can be obtained.

The resin composition of the present invention must be contained in the range of 50 to 600 parts by weight of the water-resistant aluminum nitride powder per 100 parts by weight of the resin, more preferably 100 to 600 parts by weight.
A range of 400 parts by weight is preferred. If the water-resistant aluminum nitride powder is less than 50 parts by weight, the desired thermal conductivity cannot be obtained, which is not preferable. If the amount exceeds 600 parts by weight, the desired thermal conductivity can be obtained, but the physical properties of the resin deteriorate, which is not preferable.

In the case where the heat conductive resin composition of the present invention is used as a molding material, a known method can be used. For example, a method in which a predetermined amount of a resin and water-resistant aluminum nitride powder are uniformly mixed with a mixer or the like, followed by mixing with a hot roll, followed by cooling and solidifying and pulverizing to an appropriate size. For rubbery substances of
A method in which a rubber-like substance such as silicon rubber is dissolved in a solvent, a predetermined amount of water-resistant aluminum nitride is added, and a vulcanizing agent or a catalyst is added to the obtained slurry. Further, since the water-resistant aluminum nitride powder of the present invention has good dispersibility in a resin, the water-resistant aluminum nitride can be evenly dispersed in the resin by kneading a high-viscosity resin with a kneader or the like.

Further, other additives such as silica, alumina, boron nitride and a flame retardant may be added to the resin composition of the present invention.

Since the resin composition of the present invention has excellent thermal conductivity, it is useful in fields requiring heat radiation. For example, it is used as a sealing material, a package material, an adhesive for electronic components, an insulating protective film, a molding material for a laminated substrate based on the composition of the resin composition of the present invention, and the like.

[0039]

The present invention will be described below with reference to examples. The percentages and parts are expressed on a weight basis unless otherwise specified. Production Example of Aluminum Nitride Powder Production Example 1 56.8 parts of a 2.4% orthophosphoric acid aqueous solution (orthophosphoric acid 1.
(4 parts, water 55.4 parts), 2% of water-repellent silica with respect to the aluminum nitride powder was previously slurried with methanol and dispersed in an orthophosphoric acid aqueous solution. Next, aluminum nitride powder (average particle size: 1) was added to the above-mentioned orthophosphoric acid solution.
μm), and kneaded with a 5 L kneader to form a paste, which was then treated at 30 ° C. for 30 minutes. This mixture was dried at 120 ° C. for 8 hours, and after drying, pulverized by a jet mill to obtain a water-resistant aluminum nitride powder.

Production Examples 2 and 3 Aluminum nitride powder was obtained in the same manner as in Example 1 except that the amount of water-repellent silica was changed to 5% and 10%.

Production Example 4 Same as Example 1 except that the 2.4% aqueous solution of orthophosphoric acid was changed to 60.5 parts of a 6.8% aqueous solution of orthophosphoric acid (4.1 parts of orthophosphoric acid, 56.4 parts of water). Water-resistant aluminum nitride powder was obtained by the above method.

Production Example 5 A method similar to that of Example 1 except that the 2.4% aqueous solution of orthophosphoric acid was changed to 69.7 parts of an aqueous solution of 15.8% orthophosphoric acid (11 parts of orthophosphoric acid and 58.7 parts of water). Thus, a water-resistant aluminum nitride powder was obtained.

Production Examples 6 and 7 Water-resistant aluminum nitride powder was obtained in the same manner as in Example 1 except that the fluidity improver was changed to alumina and boron nitride.

Production Example 8 100 parts of aluminum nitride powder (average particle size: 1 μm) was added to 60.5 parts of a 6.8% orthophosphoric acid aqueous solution (4.1 parts of orthophosphoric acid, 56.4 parts of water) using a 5 L kneader. It was made into a kneaded paste and was treated at 30 ° C. for 30 minutes. This mixture was dried at 120 ° C. for 8 hours, and after drying, pulverized by a jet mill to obtain a water-resistant aluminum nitride powder. Furthermore, 2% of water-repellent silica was added to the water-resistant aluminum nitride powder, and a ball made of alumina was put into a porcelain pot having a capacity of 1 L, and mixed and crushed at 120 rotations for 1 hour.
A water-resistant aluminum nitride powder was obtained.

Production Example 9 56.8 parts of a 2.4% aqueous solution of orthophosphoric acid (orthophosphoric acid 1.
(4 parts, water 55.4 parts), 2% of water-repellent silica with respect to the aluminum nitride powder was previously slurried with methanol and dispersed in an orthophosphoric acid aqueous solution. Next, aluminum nitride powder (average particle size: 1) was added to the above-mentioned orthophosphoric acid solution.
μm), and kneaded with a 5 L kneader to form a paste, which was then treated at 30 ° C. for 30 minutes. The mixture was dried at 120 ° C. for 8 hours, heat-treated at 300 ° C. for 5 hours, and then pulverized by a jet mill to obtain a water-resistant aluminum nitride powder.

Production Example 10 Production Example 9 except that the amount of water-repellent silica was changed to 3%.
Water-resistant aluminum nitride powder was obtained in the same manner as described above.

Production Examples 11 to 12 The water-resistant aluminum nitride powder obtained in Production Examples 9 to 10 was
After washing with pure water at 00 ° C, filtration and drying, the mixture was pulverized with a jet mill to obtain a water-resistant aluminum nitride powder.

Production Example 13 The same procedure as in Production Example 1 was carried out except that the water-repellent silica was not used.

Production Examples 14 and 15 The same procedures as in Production Examples 4 and 5 were carried out except that the water-repellent silica of Production Examples 4 and 5 was omitted.

Example 1 To 100 parts of silicon rubber, 80 parts of the water-resistant aluminum nitride powder having improved fluidity obtained in Production Example 1 was kneaded with a kneader for 15 minutes to prepare a silicon rubber composition containing water-resistant aluminum nitride. I got something. The obtained resin composition,
Extrusion was performed through a 150 mesh strainer, but no agglomerates were found that did not pass through the strainer. As a result of measuring the thermal conductivity of this molded body using a laser flash method thermal constant measuring apparatus, 3.5 W / mK was obtained.
Met. This molded product and pure water (molded product / pure water = 1/8 (weight ratio)) are put in a stainless steel container, and the container is sealed.
For 3 days, and the pH and electric conductivity of the recovered liquid were measured to evaluate the water resistance and the elution of ionic components. Further, as a result of observing the molded body after the test, no particular change was observed in the molded body.

Examples 2 to 6 The addition amount of the water-resistant aluminum nitride powder having improved fluidity obtained in Production Example 1 was 100 parts, 200 parts, 300 parts,
A molded product was obtained in the same manner as in Example 1 except that the amount was changed to 400 parts and 550 parts. Evaluation was performed in the same manner as in Example 1, and the evaluation results are shown in Table 1.

Examples 7 to 17 Example 1 was repeated except that the water-resistant aluminum nitride powder obtained in Production Examples 2 to 12 was used, and the addition amount was changed to 200 parts.
A molded article was obtained in the same manner as described above. Evaluation was performed in the same manner as in Example 1, and the evaluation results are shown in Table 1.

Example 18 200 parts of the water-resistant aluminum nitride powder of Production Example 1 was mixed with 100 parts of the epoxy resin using a Henschel mixer. The obtained mixture was heated at 180 ° C. for 25 minutes by a heating press, and further cured at 200 ° C. for 2 hours to obtain a molded body. As a result of rolling the epoxy resin composition, no aggregate was observed in the resin. It was 5.6 W / mK as a result of measuring the thermal conductivity of this molded body using a laser flash method thermal constant measuring apparatus. This molded product and pure water (molded product / pure water = 1/8 (weight ratio)) were put in a stainless steel container, sealed, and heated at 120 ° C. for 3 days.
H and electric conductivity were measured to evaluate water resistance and dissolution of ionic components. Further, as a result of observing the molded body after the test, no particular change was observed in the molded body.

Examples 19 to 23 The same as Example 18 except that the addition amount of the water-resistant aluminum nitride powder obtained in Production Example 1 was changed to 80 parts, 100 parts, 300 parts, 400 parts and 550 parts. A molded article was obtained by the method. Evaluation was performed in the same manner as in Example 1, and the evaluation results were shown in Table 1.
Shown in

Example 24 200 parts of the water-resistant aluminum nitride powder of Production Example 1 was mixed with 100 parts of a polyamide resin using a Henschel mixer.
After sufficiently drying at 0 ° C, the mixture was kneaded at 230 ° C with a twin-screw extruder to form pellets. The pellet is dried again at 80 ° C.
Injection molding was performed at 250 ° C. to obtain a molded body. As a result of rolling the polyamide resin composition, no aggregate was found in the resin. As a result of measuring the thermal conductivity of the molded body using a laser flash method thermal constant measuring apparatus, 5.5 W / m was obtained.
It was K. A stainless steel container was charged with the molded article and pure water (molded article / pure water = 1/8 (weight ratio)), and sealed,
The solution was heated at a temperature of 3 ° C. for 3 days, and the pH and electric conductivity of the collected solution were measured to evaluate the water resistance and the dissolution of ionic components.
Further, as a result of observing the molded body after the test, no particular change was observed in the molded body.

Comparative Example 1 A molded product was obtained in the same manner as in Example 1 except that the amount of the water-resistant aluminum nitride powder obtained in Production Example 1 was changed to 30 parts. Evaluation was performed in the same manner as in Example 1, and the evaluation results are shown in Table 2.

Comparative Examples 2 to 4 Water-resistant aluminum nitride-containing silicon rubber compositions were obtained in the same manner as in Example 1, except that the water-resistant aluminum nitride powders obtained in Production Examples 13 to 15 were used. The resulting resin composition was extruded through a 150-mesh strainer, and aggregates were found that were too small to pass through the strainer. When the aggregates were identified by X-ray diffraction,
It was confirmed to be aluminum nitride. This molded product and pure water (molded product / pure water = 1/8 (weight ratio)) are put in a stainless steel container, sealed, heated at 120 ° C. for 3 days, and the pH and electric conductivity of the recovered liquid are measured. Then, the water resistance and the dissolution property of the ionic component were evaluated. Further, as a result of observing the molded article after the test, changes such as discoloration and a rough surface of the molded article are observed, and deterioration of the molded article is observed. Further, the thermal conductivity was measured in the same manner as in Example 1, and is shown in Table 2.

Comparative Examples 5 to 7 Except that the aluminum nitride powders obtained in Production Examples 13 to 15 were used, molded articles were obtained in the same manner as in Example 18. As a result of rolling the epoxy resin composition, aggregates were observed in the resin. When the aggregate was identified by an X-ray diffraction method, it was confirmed that the aggregate was aluminum nitride. This molded product and pure water (molded product / pure water = 1/8 (weight ratio)) are put in a stainless steel container, sealed, heated at 120 ° C. for 3 days, and the pH and electric conductivity of the recovered liquid are measured. Then, the water resistance and the dissolution property of the ionic component were evaluated. Further, as a result of observing the molded article after the test, changes such as discoloration and a rough surface of the molded article are observed, and deterioration of the molded article is observed. Further, the thermal conductivity was measured in the same manner as in Example 1, and is shown in Table 2.

[0059]

[Table 1]

[0060]

[Table 2] ：: No aggregate in resin ×: Aggregate in resin

[0061]

The resin composition of the present invention is uniformly dispersed in the resin by using the water-resistant aluminum nitride powder, so that a higher quality heat conductive resin composition than before can be obtained. The water-resistant aluminum nitride powder used in the present invention has excellent water resistance and low elution of ionic components, so that even when used under high temperature and high humidity, the thermal conductivity is reduced, insulation breakdown and circuit corrosion are caused. And a product with higher reliability than the conventional product can be obtained. Since the resin composition according to the present invention has excellent thermal conductivity, it is useful as a sealing material for electronic components requiring heat dissipation, an adhesive for electronic components, and the like. It is also useful as a material for forming a laminated substrate based on the composition of the resin composition of the present invention.

──────────────────────────────────────────────────の Continued on the front page (51) Int.Cl. ⁶ Identification code FI C08K 5/521 C08K 5/521 C08L 27/12 C08L 27/12 61/06 61/06 63/00 63/00 67/00 67 / 00 69/00 69/00 71/12 71/12 75/04 75/04 77/00 77/00 79/04 79/04 83/04 83/04 C09C 1/40 C09C 1/40

Claims (9)

[Claims] 1. Excellent water resistance characterized by containing 50 to 600 parts by weight of a water-resistant aluminum nitride powder containing a phosphoric acid compound in an aluminum nitride powder and a fluidity improver based on 100 parts by weight of a resin. High thermal conductive resin composition. 2. The resin is an epoxy resin, a silicone resin, a silicone rubber, a polyimide resin, a polycarbonate resin, a polyamide resin, a polyphenylene oxide resin,
The high thermal conductive resin composition according to claim 1, which is a urethane resin, a phenol resin, a polyester resin, or a fluororesin. 3. The highly thermally conductive resin composition according to claim 1, wherein the water-resistant aluminum nitride powder has a phosphoric acid compound content of 0.1 to 10% by weight in terms of P ₂ O ₅ . 4. The high thermal conductivity according to claim 1, wherein the water-resistant aluminum nitride powder contained in the resin composition is obtained by treating the aluminum nitride powder with a phosphate compound in the presence of water and mixing a fluidity improver. Resin composition. 5. A water-resistant aluminum nitride powder contained in a resin composition, wherein the aluminum nitride powder is treated with a phosphate compound in the presence of water, and a dispersant is added. The highly thermally conductive resin composition according to claim 1, which is obtained by mixing an inorganic powder having a group. 6. The highly thermally conductive resin composition according to claim 1, wherein the fluidity improver is an inorganic powder having a lipophilic group on the surface. 7. The fluidity improver comprises silica, alumina,
The highly thermally conductive resin composition according to any one of claims 1 to 3, wherein the composition is at least one selected from the group consisting of titania and boron nitride. 8. The method according to claim 1, wherein the flow improver is added in an amount of 0.1 to 10% by weight based on the aluminum nitride powder.
4. The highly thermally conductive resin composition according to any one of items 3 to 3. 9. The method according to claim 1, wherein the aluminum nitride powder is obtained by a reaction between an organic aluminum compound and ammonia.
The high thermal conductive resin composition according to any one of Items 4 to 4.