CN109502561B - Method for synthesizing aluminum nitride by directly burning magnesium-aluminum alloy particles in air - Google Patents
Method for synthesizing aluminum nitride by directly burning magnesium-aluminum alloy particles in air Download PDFInfo
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- CN109502561B CN109502561B CN201811576655.8A CN201811576655A CN109502561B CN 109502561 B CN109502561 B CN 109502561B CN 201811576655 A CN201811576655 A CN 201811576655A CN 109502561 B CN109502561 B CN 109502561B
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- C01B21/00—Nitrogen; Compounds thereof
- C01B21/06—Binary compounds of nitrogen with metals, with silicon, or with boron, or with carbon, i.e. nitrides; Compounds of nitrogen with more than one metal, silicon or boron
- C01B21/072—Binary compounds of nitrogen with metals, with silicon, or with boron, or with carbon, i.e. nitrides; Compounds of nitrogen with more than one metal, silicon or boron with aluminium
- C01B21/0722—Preparation by direct nitridation of aluminium
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- C01B21/0612—Binary compounds of nitrogen with metals, with silicon, or with boron, or with carbon, i.e. nitrides; Compounds of nitrogen with more than one metal, silicon or boron with alkaline-earth metals, beryllium or magnesium
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- C01F5/00—Compounds of magnesium
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- C01F5/04—Magnesia by oxidation of metallic magnesium
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- C01F7/00—Compounds of aluminium
- C01F7/02—Aluminium oxide; Aluminium hydroxide; Aluminates
- C01F7/16—Preparation of alkaline-earth metal aluminates or magnesium aluminates; Aluminium oxide or hydroxide therefrom
- C01F7/162—Magnesium aluminates
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Abstract
The invention provides a method for synthesizing aluminum nitride by directly burning magnesium-aluminum alloy particles in air, which comprises the following steps: the method comprises the following steps of freely accumulating magnesium-aluminum alloy powder on an asbestos net, placing the asbestos net in an air environment, using an external heating source for ignition, removing the heating source after the alloy is fully ignited, enabling the alloy to be self-propagating and combusted, obtaining blocky aluminum nitride on the lower layer of a combustion product after the combustion is finished, and grinding the blocky aluminum nitride by using a ball-milling device to obtain the aluminum nitride powder. The invention saves a large amount of energy by utilizing the characteristics of low ignition temperature of the raw materials in the air and self-sustained combustion. The invention can be carried out in air environment at normal temperature and normal pressure, and has low process requirement. The prepared final product aluminum nitride has uniform color, good crystallization and high conversion rate.
Description
Technical Field
The invention relates to the field of preparation of aluminum nitride, in particular to a method for synthesizing aluminum nitride by directly burning magnesium-aluminum alloy particles in air.
Background
Aluminum nitride has excellent properties and is widely used in the fields of semiconductors, ceramics, optoelectronics, and the like. The traditional method for synthesizing aluminum nitride mainly comprises a carbothermic method, a direct nitriding method, a self-propagating high-temperature synthesis method and the like. For the direct nitridation method and the self-propagating high-temperature synthesis method, the reaction often needs to be performed under high pressure due to the existence of a nitrogen gas permeation energy barrier. Moreover, the reaction has strict requirements on the nitriding temperature.
For the carbothermic reduction method, pure aluminum nitride can be obtained, but the reduction temperature is generally above 1000 ℃, and because excessive carbon powder is used in the synthesis process, the aluminum nitride prepared by the carbothermic reduction method needs to be subjected to decarburization treatment, the synthesis is time-consuming and complex in process, and the requirement on equipment is high.
Disclosure of Invention
The invention aims to provide a method for synthesizing aluminum nitride by directly burning magnesium-aluminum alloy particles in air, which solves the problems of high synthesis temperature, long time consumption, low conversion efficiency, complex process and the like in the existing method.
The technical scheme for realizing the purpose of the invention is as follows:
a method for synthesizing aluminum nitride by directly burning magnesium-aluminum alloy particles in air comprises the following steps:
(a) low-temperature synthesis: freely accumulating the raw material magnesium-aluminum alloy powder on a sample table, igniting by using an external heating source, removing the heating source after the alloy is fully ignited, enabling the combustion to be self-propagating, and obtaining the massive aluminum nitride after the combustion is finished;
(b) and (3) product separation: separating the upper magnesium oxide layer from the lower aluminum nitride layer by using high-pressure air and a brush; drying the product at 50-120 deg.c for 1-5 hr to obtain high purity aluminum nitride;
(c) crushing a product: and grinding the block aluminum nitride synthesized by combustion in a ball mill to obtain powdery aluminum nitride.
Further, in the step (a), the magnesium-aluminum alloy is spherical particles, the mass ratio of magnesium to aluminum in the alloy is 50:50, and Al is mainly used12Mg17The phases exist in the form.
Further, in the step (a), the sample stage is an asbestos cloth.
Further, in the step (a), the sample is in an air environment and is combusted at normal temperature and normal pressure.
Further, in step (a), the heating source is any heat source capable of igniting the sample.
Further, the heat source for igniting the sample may be an n-heptane flame, an ethane flame, or an electric heating wire.
Further, in the step (b), the drying oven is a common air-blast drying oven, and the maximum drying temperature is 300 ℃.
Compared with the prior art, the invention has the following remarkable advantages:
1. the invention uses spherical Mg-Al alloy powder (Al)12Mg17) The high-purity AlN crystal can be synthesized by directly burning the raw material in the air.
2. The invention does not need high temperature environment, because the ignition temperature of the magnesium-aluminum alloy is lower (494.4 ℃), once the magnesium-aluminum alloy is ignited, the magnesium-aluminum alloy does not need to be heated by an external heat source, and the heat generated by combustion is enough to maintain the combustion, so that the synthesis can be directly carried out in the normal temperature environment; the synthesis can be carried out directly in air conditions without the need to use an additional nitrogen source or high purity nitrogen.
3. The Al in the alloy prepared by the preparation method can be completely converted into AlN, so that the conversion rate of the aluminum is greatly improved; the combustion product is composed of MgO and AlN, obvious layering occurs, high-pressure gas and a brush can be used for separating the MgO and the AlN, and the synthesis steps are simplified.
Drawings
Fig. 1 is a diagram of the products of direct combustion of magnesium-aluminum alloy in air.
Fig. 2 is an SEM image of the synthesized aluminum nitride.
FIG. 3 is an XRD pattern of the combustion products, wherein (a) is magnesium oxide taken from the upper layer and (b) is aluminum nitride taken from the lower layer.
Detailed Description
The following examples further illustrate the invention in detail, but are not to be construed as limiting the invention in any way.
The magnesium-aluminum alloy (the content is more than 99 percent) used in the embodiment is purchased from Shandong Tangshan Weihao magnesium powder limited company, and uniform spherical alloy particles are finally obtained by adopting an atomization forming process.
Example 1: weighing 5 g of particles with the particle size distribution of 100-150 meshes and the mass ratio of 50:50 (mainly Al)12Mg17Phase form) is deposited on an asbestos gauze, and the alloy is heated and ignited from below the asbestos gauze by using an alcohol burner in an air environment. After the alloy is fully ignited, the heating source is removed, after the combustion is stopped, the sample is cooled, the blocky aluminum nitride is cleaned by using high-pressure gas and a brush until the magnesium oxide is completely removed, and the blocky aluminum nitride can be obtained after drying for two hours in a blast drying oven at the temperature of 80 ℃. The aluminum nitride block was ground for 10 minutes at 500rpm using a ball mill to obtain aluminum nitride powder.
Example 2: weighing 5 g of particles with the particle size of about 325 meshes and the mass ratio of 50:50 (mainly Al)12Mg17In phase form) of magnesium-aluminum alloy, which is freely deposited on asbestos meshes, in the airIgniting by using a heating wire in a gas environment, after the alloy is fully combusted and cooled, cleaning the blocky aluminum nitride by using high-pressure gas and a brush until magnesium oxide is completely removed, and drying in a blast drying oven at 100 ℃ for 1 hour to obtain the blocky aluminum nitride. The aluminum nitride powder was obtained by grinding the bulk aluminum nitride at 500rpm for 10 minutes using a ball mill.
Example 3: weighing 5 g of magnesium-aluminum alloy with the particle size distribution of 100-150 meshes and the mass ratio of 50:50, placing the magnesium-aluminum alloy into a ceramic crucible, placing the ceramic crucible into a high-temperature resistance furnace in an air environment, and heating and igniting the alloy at the heating rates of 10 ℃/min, 20 ℃/min and 40 ℃/min by using a programmed heating method. To obtain magnesium oxide and MgAl2O4A mixture of (a).
Example 4: weighing 5 g of magnesium-aluminum alloy with the particle size distribution of 100-150 meshes and the mass ratio of 80:20, freely stacking the magnesium-aluminum alloy on an asbestos net, and heating and igniting the alloy from the lower part of the asbestos net by using an alcohol blast lamp in an air environment. After the alloy was fully ignited, the heating source was removed, the combustion was stopped, and after the sample was cooled, the bulk aluminum nitride was cleaned with high pressure gas and a brush until the magnesium oxide was completely removed, and dried in a forced air drying oven at 80 ℃ for two hours. So as to obtain the mixture of simple substance aluminum and aluminum nitride.
In conclusion, the Al is mainly contained in the 50:50 magnesium-aluminum alloy12Mg17The phase exists, magnesium and aluminum are uniformly distributed in each alloy particle, and the preferential reaction of magnesium and oxygen in the synthesis process enables aluminum to react only with nitrogen. The oxidation of magnesium on the one hand inhibits the reaction of aluminium with oxygen and on the other hand the heat generated by its combustion further promotes the nitriding of aluminium. Meanwhile, the gasification and diffusion of magnesium are helpful to break the aluminum nitride solid coating formed on the particle surface in the synthesis process to be thin, so that the aluminum in the alloy particles can be completely nitrided. Whereas for the 80:20 magnesium-aluminum alloy, the aluminum in the alloy exists mainly in the form of simple aluminum, and the combustion of magnesium cannot promote the nitridation of aluminum as in the 50:50 magnesium-aluminum alloy. Meanwhile, the oxidation mechanism of the magnesium-aluminum alloy is influenced by the heating rate, and MgAl is mainly generated in the alloy at a lower heating rate2O4And MgO, so choosing the appropriate heating method and sample stage has an important influence on the synthesis. In the invention, the asbestos cloth is selected as the sample table, and the sample is quickly ignited by using the high-temperature heat source, so that the generation of high-purity aluminum nitride is ensured.
Claims (5)
1. A method for synthesizing aluminum nitride by directly burning magnesium-aluminum alloy in air is characterized by comprising the following steps:
(a) low-temperature synthesis: freely accumulating the raw material magnesium-aluminum alloy powder on a sample table, igniting by using an external heating source, removing the heating source after the alloy is fully ignited, enabling the combustion to be self-propagating, and obtaining the massive aluminum nitride after the combustion is finished;
(b) and (3) product separation: separating the upper magnesium oxide layer from the lower aluminum nitride layer by using high-pressure air and a brush; drying the product at 50-120 deg.c for 1-5 hr to obtain high purity aluminum nitride;
(c) crushing a product: grinding the block aluminum nitride synthesized by combustion in a ball mill to obtain powdery aluminum nitride;
in the step (a), the magnesium-aluminum alloy is spherical particles, the mass ratio of magnesium to aluminum in the alloy is 50:50, and Al is mainly used12Mg17The phases exist in the form;
in the step (a), the sample is in an air environment and is combusted at normal temperature and normal pressure.
2. The method of claim 1, wherein in step (a), the sample stage is an asbestos cloth.
3. The method of claim 1, wherein in step (a), the heat source is any heat source capable of igniting the sample.
4. The method of claim 3, wherein the heat source capable of igniting the sample is an n-heptane flame, an ethane flame, or an electric heating wire.
5. The method of claim 1, wherein in step (b), the drying oven used for drying is a conventional forced air drying oven with a maximum drying temperature of 300 ℃.
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| CN201811576655.8A CN109502561B (en) | 2018-12-23 | 2018-12-23 | Method for synthesizing aluminum nitride by directly burning magnesium-aluminum alloy particles in air |
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Non-Patent Citations (2)
| Title |
|---|
| "Study of aluminum nitride formation by superfine aluminum powder combustion in air";Alexander Gromov等;《Journal of the European Ceramic Society》;20031118;第24卷(第9期);2879-2884 * |
| "镁铝合金的特性及在富燃料固体推进剂中的应用";肖秀友等;《中国宇航学会固体火箭推进第22届年会论文集（推进剂分册）》;20051031;175-178 * |
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