JP3417885B2 - Aluminum nitride powder - Google Patents

Description

DETAILED DESCRIPTION OF THE INVENTION [0001] TECHNICAL FIELD The present invention relates to aluminum nitride powder.
Grease or grease as a heat dissipation material for electronic components.
Nitriding with excellent water resistance, suitable for filling in synthetic rubber
Related to aluminum powder. [0002] 2. Description of the Related Art Many electronic components generate heat during use.
In order for the electronic components to function properly,
It is necessary to remove heat from the child parts. So, high
Aluminum nitride having thermal conductivity and electrical insulation,
It is expected to be applied as a heat dissipation material for electronic components
You. In this case, the form of use is as a molded product or grease.
And various forms such as synthetic rubber fillers. [0003] However, aluminum nitride is water-resistant.
Poor, especially in the case of powder, even when left in the air
Decomposition progresses gradually, producing ammonia and aluminum
To hydroxide. Therefore, aluminum nitride powder
Is used, for example, as a filler for high heat dissipation of resin
In this case, poor water resistance becomes a problem. Therefore, conventionally, the water resistance of aluminum nitride has been improved.
To improve the properties, organic polymer is converted to aluminum nitride powder.
Coating on powder surface or oxidizing aluminum nitride powder surface
To provide an aluminum oxide layer, and do not use this as a protective film.
Which attempts have been made. Also, JP-A-4-32150
No. 6 discloses an organosilane oligomer and a silanol.
Reaction with a polyorganosiloxane having a group using a catalyst
To coat the surface of aluminum nitride powder
A technique to do this has also been proposed. However, these
The water resistance of aluminum nitride can also be improved by the shifting method.
I couldn't make it clear. [0005] SUMMARY OF THE INVENTION The present inventors have found that
Investigations were made to improve the water resistance of luminium.
As a result, certain organosilanes or partially hydrolyzed condensates thereof
By treating the surface of aluminum nitride with
Aluminum nitride powder with excellent water resistance
The inventors have found out what can be done and arrived at the present invention. Therefore, the present invention
The purpose is to be a water-resistant material suitable as a filler
To provide aluminum nitride powder with excellent heat resistance.
You. [0006] SUMMARY OF THE INVENTION The above objects of the present invention are as follows.
General formula R¹ _aR² _bSi (OR³)_4-abRepresented by
Organosilanes and / or their partially hydrolyzed condensates
Therefore, aluminum nitride characterized by being surface-treated
Powder (however, in the above formula, R¹Is the carbon number10~ 15
An alkyl group of R²Is unsubstituted or substituted having 1 to 8 carbon atoms
Monovalent hydrocarbon group, R³Is an alkyl group having 1 to 6 carbon atoms, a
Is an integer of 1-3, b is an integer of 0-2, a + b is an integer of 1-3
Is an integer). [0007] BEST MODE FOR CARRYING OUT THE INVENTION As a surface treatment agent in the present invention,
R in the above general formula of the organosilane used¹of
Specific examples include, for example, a decyl group, a dodecyl group,
Radecyl group, pentadecyl group and the like can be mentioned. Carbon number
10Smaller than treated aluminum nitride powder
If the water is not enough and it is larger than 15, the organosilane will
Since it solidifies at room temperature, it is inconvenient to handle, grease and
When filled in a synthetic rubber, the low-temperature characteristics deteriorate. Ma
A is 1, 2 or 3, but especially 1
preferable. Further, R in the above general formula²Has 1 to 1 carbon atoms
8 is a saturated or unsaturated monovalent hydrocarbon group.
Examples of such groups include an alkyl group, a cycloalkyl group, and an alky group.
A kenyl group and the like can be mentioned. R²As a specific example of
Is, for example, methyl, ethyl, propyl, hex
Alkyl group such as octyl group, cyclopentyl group,
Cyclohexyl group such as cyclohexyl group, vinyl group,
An alkenyl group such as a ryl group, an aryl group such as a phenyl group,
2-phenylethyl group, 2-methyl-2-phenylethyl
Aralkyl groups such as
Group, 2- (perfluorobutyl) ethyl group, p-chloro
Halogenated hydrocarbon groups such as a phenyl group are exemplified. Book
Among these, a methyl group is particularly preferred in the invention.
No. Also, R³As an alkyl group having 1 to 6 carbon atoms
Among them, a methyl group and an ethyl group are particularly preferable. Note that R
¹, R², R³Are two or more as shown below.
In some cases. An organosilane component represented by the above general formula
Examples of the body include the following. C₁₀H₂₁Si (OCH₃)₃, C₁₂H₂₅Si
(OCH₃)₃, C₁₀H ₂₁Si (CH₃) (OCH
₃)₂, C₁₀H₂₁Si (C₆H₅) (OC
H₃)₂, C₁₀H₂₁Si (CH₃) (COCH₃)
₂, C₁₀H₂₁Si (CH = CH₂) (OC
H₃)₂, C₁₀H₂₁Si (CH₂CH₂CF₃)
(OCH ₃)₂ The organosilane represented by the above general formula is
0.1 to 30 parts per 100 parts by weight of aluminum nitride powder
It is preferable to use parts by weight, particularly 0.5 to 10 parts by weight
It is preferable to use parts. From 0.1 parts by weight
If less, water resistance will be poor and 30 parts by weight
Even if the amount is large, the effect does not increase and it is uneconomical. [0011] Aluminum nitride powder used in the present invention
Has a generally hexagonal or wurtzite-type crystal structure
It is a group III-V nitride and its appearance is white to off-white.
The particle shape varies depending on the manufacturing method, but it is irregular-shaped to spherical powder.
is there. In the present invention, the average particle size is 0.1 ~ 100μ
Aluminum nitride powder in a wide range of m
However, to obtain a uniform molded body, grease, synthetic rubber, etc.
For this reason, it is preferable to use one with a thickness of 1 to 10 μm.
It is particularly preferable to use one having a size of 2 to 5 μm.
The specific surface area is 0.1-100m²/ G range
Can be used for uniform molding, grease, synthetic rubber
1 to 10m to get²/ G
Is preferred, especially 2 to 5 m²/ G
Is preferred. A method for producing such aluminum nitride powder and
The metal aluminum powder and nitrogen or ammonia
Direct nitridation method that directly reacts with carbon, mixing of alumina and carbon
Heat powder under nitrogen or ammonia atmosphere to reduce
Alumina reduction method that simultaneously performs and nitriding, or aluminum
Direct reaction between nitrogen vapor and nitrogen, AlCl
₃・ NH₃And a production method such as thermal decomposition. To the manufacturing method
More chemical composition (impurities), particle size and shape, particle size distribution, etc.
Of the aluminum nitride used in the present invention
Minium powder used in any method can be used.
Can mix these different recipes
May be used. The surface-treated aluminum nitride of the present invention
Can be produced by a known method. For example, nitriding
Aluminum and organosilane or its partial water content
Demolition, trimix, twin mix, planetary
Mixers (both are registered trademark of mixers manufactured by Inoue Manufacturing Co., Ltd.)
Mark), Ultra Mixer (mixer manufactured by Mizuho Industry Co., Ltd.)
Registered trademark), Hibis Dispermix (special machine chemical
Mixing using a mixer such as a registered trademark of Mixer Co., Ltd.)
I do. In this case, if necessary, increase the temperature to 50 to 150 ° C.
May be heated. When mixing, toluene and xylene
Oil, petroleum ether, mineral spirit, isoparaffin
Solvent such as isopropyl alcohol, ethanol, etc.
May be. When these solvents are used, after mixing,
It is preferable to remove the solvent using a vacuum device or the like. This
Aluminum nitride powder of the present invention produced as described above
Can be used as filler for grease or rubber sheet, or
As a high-purity aluminum nitride compact
Can also be used. [0015] According to the present invention, the aluminum nitride of the present invention is significantly resistant.
Aqueous solution is improved and ammonia is generated due to hydrolysis reaction
Can be used under high humidity, and thermoelectric
Good conductivity, especially suitable as filler for heat dissipation material
It is. [0016] The present invention will be described in more detail with reference to the following examples.
However, the present invention is not limited by this.
The moisture resistance of aluminum nitride powder was evaluated as follows.
I went. [0017]Moisture resistance test Aluminum nitride powder in a stopperable 250ml plastic container
After adding 5 g of powder and 95 g of water, stopper and shaker
Shake (room temperature) for 48 hours. Then filter using filter paper.
The solution is collected and its pH is measured by Horiba, Ltd.
(Model F-15). Embodiment 1 FIG. Organosila of component (A-1)
10 g of aluminum nitride powder (B-1) (undefined
Shape, average particle size 2.0 μm, specific surface area 4.0 m²/ G)
1000g to 5 liter planetary mixer (made by Inoue
And then stirred and mixed at room temperature for 30 minutes.
A surface-treated aluminum nitride powder was obtained. P after moisture resistance test
H was 7.9. Embodiments 2 and 3 Olga of component (A-1)
Example 1 was the same as Example 1 except that the blending amount of the silane was as shown in Table 1.
In the same manner, a surface-treated aluminum nitride powder was obtained. This
The pH values after these moisture resistance tests are as shown in Table 1. [0020] [Table 1] Embodiments 4-6. Used in Example 1 (A-
The organosilane of 1) was converted to (A-2) and (A-
3) and (A-4) except that the organosilane was changed to
Surface-treated aluminum nitride powder in exactly the same manner as in Example 1.
I got the end. The pH values after these moisture resistance tests were as shown in Table 1.
It is. Comparative Example 1 Aluminum nitride used in the above example
Moisture resistance test of untreated titanium powder (B-1)
Was performed, the pH was 11.5 as shown in Table 1.
there were. Comparative Example 2 Aluminum nitride powder (B-
1) is heat-treated in an oxygen atmosphere at 500 ° C. for 30 minutes,
Powder having an aluminum oxide layer formed on the surface (B-2)
I got Example of the obtained aluminum nitride powder
Table 1 shows the results of a moisture resistance test performed in exactly the same manner as in Example 1.
Thus, the pH was 11.5. Comparative Examples 3.4 and 5. Used in Example 1
(A-1) the organosilane of (A-5),
(A-6) and (A-7) were changed to organosilanes
Outside, the surface-treated aluminum nitride was treated in exactly the same manner as in Example 1.
Powder was obtained. A moisture resistance test was performed on the obtained powder.
As a result, as shown in Table 1, the pH was 11.
3, 10.5 and 9.3.

────────────────────────────────────────────────── ─── Continuing from the front page (72) Inventor Kenichi Isobe 1-10 Hitomi, Matsuida-cho, Usui-gun, Gunma Prefecture Shin-Etsu Chemical Co., Ltd. Silicone Electronics Materials Research Laboratory (56) References JP-A-4-321506 (JP, A) JP-A-3-287654 (JP, A) JP-A-7-315813 (JP, A) (58) Fields investigated (Int. Cl. ⁷ , DB name) C09C 3/12 C08K 3 / 28 C08K 9/06 C09C 1/40 C01B 21/072

Claims (1)

(57) [Claims] [Claim 1] The general formula R ¹ _a R ² _b Si (OR ³ )
_An aluminum nitride powder characterized by being surface-treated with an organosilane represented by _4-ab and / or a partial hydrolyzed condensate thereof;
¹ is an alkyl group having 10 to 15 carbon atoms, and R ² is an alkyl group having 1 carbon atom.
An unsubstituted or substituted monovalent hydrocarbon group of 8 to 8, R ³ is an alkyl group having 1 to 6 carbon atoms, a is an integer of 1 to 3, b is an integer of 0 to 2, and a + b is an integer of 1 to 3 It is.