CN110104620B - Method for preparing aluminum nitride nano powder by using sol-gel method - Google Patents
Method for preparing aluminum nitride nano powder by using sol-gel method Download PDFInfo
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- CN110104620B CN110104620B CN201910440513.7A CN201910440513A CN110104620B CN 110104620 B CN110104620 B CN 110104620B CN 201910440513 A CN201910440513 A CN 201910440513A CN 110104620 B CN110104620 B CN 110104620B
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- B—PERFORMING OPERATIONS; TRANSPORTING
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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
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- C01P2004/03—Particle morphology depicted by an image obtained by SEM
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- C01P2004/64—Nanometer sized, i.e. from 1-100 nanometer
Abstract
The invention discloses a method for preparing aluminum nitride nano powder by using a sol-gel method, which relates to the technical field of nano material preparation, wherein aluminum sol is used as an aluminum source, an organic polymer precursor is used as a carbon source, xerogel with the carbon source and the aluminum source uniformly mixed is obtained in the presence of a gelling agent and a curing agent, and gray AlN powder is obtained through pyrolysis, calcination and decarbonization; the preparation method of the aluminum nitride nano powder has low cost and simple process operation, and the prepared aluminum nitride has the particle size distribution of 30-200 nm and good dispersibility.
Description
The technical field is as follows:
the invention relates to the technical field of nano material preparation, in particular to a method for preparing aluminum nitride nano powder by using a sol-gel method.
Background art:
the aluminum nitride ceramic has a series of excellent performances such as high thermal conductivity, low dielectric constant and dielectric loss, excellent junction edge performance, high temperature resistance, chemical corrosion resistance, no toxicity, thermal expansion coefficient which can be well matched with silicon and the like; the method is widely applied to the field of electronic devices. The nanometer AlN powder has smaller granularity and high reaction activity, can reduce the densification sintering temperature, is beneficial to realizing low-temperature sintering and reduces the sintering cost of ceramics. The forming and sintering process of the aluminum nitride ceramic is not only related to the particle size of the AlN powder, but also influenced by the morphology and the particle size distribution of the AlN powder. Therefore, to prepare an aluminum nitride ceramic with good properties, it is necessary to synthesize an aluminum nitride powder with high purity, fine particle size, and good dispersibility.
Nanoscale aluminum nitride materials have more excellent properties, such as: the sintering material of the nano aluminum nitride has higher thermal conductivity and can be applied to high-energy-consumption devices; the superfine high-purity nano aluminum nitride powder can be sintered by a special process to obtain transparent aluminum nitride ceramics for preparing special optical devices.
The patent CN103072961A reports a method for preparing nano aluminum nitride, which comprises heating and melting aluminum raw material to convert it into liquid, continuously feeding into a high-temperature metal evaporator to convert the liquid aluminum into aluminum vapor, feeding into a nitriding reaction chamber through a particle former, introducing nitriding reaction gas into the nitriding reaction chamber, and reacting the nitriding gas with nano droplet-shaped aluminum to form nano aluminum nitride powder. The method relates to the liquefaction, gasification and transportation of the simple aluminum substance, and the liquefaction of the gaseous aluminum into small droplets in an industrial state, and has a complex process.
Patent CN103539088A discloses a method for preparing nano aluminum nitride, which uses aluminum nitrate and melamine as raw materials, adopts a sol-gel preparation process to prepare a precursor mixed by an aluminum source and a carbon source, and then performs carbothermic reduction on the precursor at a high temperature to prepare AlN.
Patent CN101973534A discloses a method for preparing nano aluminum nitride by low temperature combustion, which comprises mixing aluminum nitrate as aluminum source and oxidant, urea as reducing agent and combustion agent, with water-soluble carbon source according to a certain ratio, and then performing carbothermal reduction reaction at high temperature to prepare aluminum nitride. The method adopts urea as a combustion agent, the reaction process is complex, the combustion temperature is difficult to control, the particle size distribution of the aluminum nitride is wide, and the generated aluminum nitride is mostly in a flaky shape.
The invention content is as follows:
the invention aims to solve the technical problem of providing a method for preparing aluminum nitride nano powder by using a sol-gel method, which has the advantages of low cost and simple process operation, and the prepared aluminum nitride has the particle size distribution of 30-200 nm and good dispersibility.
The technical problem to be solved by the invention is realized by adopting the following technical scheme:
a method for preparing aluminum nitride nano powder by using a sol-gel method comprises the following steps:
(1) adopting aluminum sol as an aluminum source and an organic polymer precursor as a carbon source;
(2) uniformly mixing the aluminum sol and the raw materials for synthesizing the organic polymer precursor, and adding a gelling agent to adjust the pH value of the obtained mixture to 1-2;
(3) stirring the mixture to obtain stable sol in which a carbon source and an aluminum source are uniformly mixed, and cooling to room temperature;
(4) adding a curing agent into the sol at room temperature, stirring to form hydrosol, transferring the hydrosol into a drying oven for drying to obtain dry gel with uniformly mixed carbon source and aluminum source;
(5) grinding and crushing the xerogel, and pyrolyzing the xerogel in a non-oxidizing atmosphere to obtain precursor powder in which aluminum oxide and amorphous carbon are uniformly mixed;
(6) calcining the precursor powder in a flowing atmosphere, and reacting to obtain black powder;
(7) and (3) decarbonizing the black powder in an air atmosphere to obtain the offwhite AlN powder.
The aluminum sol in the step (1) is selected from alpha-Al (OH)3Sol, beta-Al (OH)3One or more of sol and AlOOH sol.
The organic polymer precursor in the step (1) is selected from one or more of phenolic resin, urea resin, melamine resin and polyvinyl alcohol.
The gelling agent in the step (2) is selected from nitric acid, hydrochloric acid, acetic acid or ammonia water.
The curing agent in the step (4) is selected from one or more of hexamethylenetetramine and polyaldehyde.
And (3) drying the oven in the step (4) at the drying temperature of 80-120 ℃.
The non-oxidizing atmosphere in the step (5) is selected from N2、Ar、N2-H2One of the mixed gases.
The flowing atmosphere in the step (6) is selected from NH3、N2At least one of (1).
The pyrolysis temperature in the step (5) is 600-800 ℃; the calcining temperature in the step (6) is 1200-1600 ℃; the carbon removal temperature in the step (7) is 600-800 ℃.
The particle size of the AlN powder in the step (7) is 30-200 nm.
The preparation principle of the invention is as follows:
Al2O3+3C+N2＝2AlN+3CO
the invention has the beneficial effects that:
(1) according to the invention, the aluminum sol and the raw materials for synthesizing the organic polymer precursor are mixed, and the organic polymer is formed by polymerization of the raw materials, so that the carbon source and the aluminum source are uniformly mixed, and the problem of nonuniform mixing of the aluminum source and the carbon source caused by rapid increase of the viscosity of a solution formed by directly adding water-soluble polymers such as polyacrylic acid and polyacrylamide as the carbon source in the prior art and dissolving in water is solved; the phenolic resin, the urea-formaldehyde resin and the melamine resin selected by the invention are not soluble in water, and the resins can not be directly added as a carbon source under the condition that water is used as a solvent, otherwise, the carbon source and an aluminum source are mixed unevenly, and finally, the nitridation reaction is incomplete.
(2) The invention adopts a gel-sol method, the sol-gel method has the advantages that the raw materials are mixed more uniformly, the added gelatinizing agent has the function of converting the formed latex into stable and uniform gel and keeping the original shape, and the control of the pH value is the necessary condition for synthesizing resin; meanwhile, the carbon source adopted by the invention belongs to resins, the resin polymer adopts two monomers as raw materials and is polymerized in a gradual polymerization mode, and the curing agent has the function of forming cross-linking between polymer chains to form a reticular polymer material so that an aluminum source is uniformly fixed in a resin reticular structure (the monomer polymerization in the gradual polymerization mode has the defect that the molecular weight of the formed polymer is possibly small, the polymer is possibly volatilized in a micromolecule mode in the high-temperature carbon forming process, the carbon forming yield is low, and the reticular structure is formed between the polymer chains by adding the curing agent so that the carbon yield is increased in the carbon forming process).
(3) The invention adopts the carbothermic method to prepare the aluminum nitride, in order to ensure that the reaction is complete and the reaction speed is accelerated, the added carbon source is excessive, and finally the decarbonization treatment is carried out.
Description of the drawings:
FIG. 1 is an XRD pattern of an aluminum nitride nanopowder prepared in example 1;
FIG. 2 is an SEM photograph of the aluminum nitride nanopowder prepared in example 1.
The specific implementation mode is as follows:
in order to make the technical means, the original characteristics, the achieved purposes and the effects of the invention easy to understand, the invention is further explained by combining the specific embodiments and the drawings.
Example 1
Weighing 100g of AlOOH sol with the mass fraction of 5%, uniformly mixing 0.1mol of phenol and 0.085mol of formaldehyde, transferring the mixture into the AlOOH sol, heating to 80 ℃, adjusting the pH to 1-2 by using 2mol/L hydrochloric acid, and magnetically stirring for 12 hours to obtain gel with a uniformly mixed aluminum source and phenolic resin; cooling to room temperature, adding 0.01mol of hexamethylenetetramine into the solution, stirring for 30min, transferring the solution to a drying oven at 120 ℃ and drying for 12h to obtain xerogel with uniformly mixed aluminum source and carbon source; xerogel on N2Keeping the temperature at 600 ℃ for 2h under the atmosphere to form carbon, and then flowing N at 1500 DEG C2Calcining for 12h under the atmosphere, and removing carbon from the calcined product for 2h in an air atmosphere at 700 ℃.
The particle size of the prepared aluminum nitride powder is 30-120 nm, and the dispersibility is good.
Example 2
Weighing 25% of Al (OH)320g of sol, 0.1mol of phenol and 0.085mol of formaldehyde are uniformly mixed and transferred to Al (OH)3Heating the sol to 85 ℃, adjusting the pH to 1-2 by using 2mol/L nitric acid, and magnetically stirring for 12 hours to obtain gel in which an aluminum source and phenolic resin are uniformly mixed; cooling to room temperature, adding 0.01mol of hexamethylenetetramine into the solution, stirring for 30min, transferring the solution to a drying oven at 100 ℃ and drying for 12h to obtain xerogel with uniformly mixed aluminum source and carbon source; xerogel on N2Keeping the temperature at 600 ℃ for 2h under the atmosphere to form carbon, and then flowing N at 1600 DEG C2Calcining for 6h under the atmosphere, and removing carbon from the calcined product for 2h in the air atmosphere at 700 ℃.
The particle size of the prepared aluminum nitride powder is 50-200 nm, and the aluminum nitride powder is well dispersed.
The foregoing shows and describes the general principles and broad features of the present invention and advantages thereof. It will be understood by those skilled in the art that the present invention is not limited to the embodiments described above, which are described in the specification and illustrated only to illustrate the principle of the present invention, but that various changes and modifications may be made therein without departing from the spirit and scope of the present invention, which fall within the scope of the invention as claimed. The scope of the invention is defined by the appended claims and equivalents thereof.
Claims (9)
1. A method for preparing aluminum nitride nano powder by utilizing a sol-gel method is characterized by comprising the following steps: the method comprises the following steps:
(1) adopting aluminum sol as an aluminum source and an organic polymer precursor as a carbon source, wherein the organic polymer precursor is selected from one of phenolic resin, urea resin and melamine resin;
(2) uniformly mixing the aluminum sol and two monomers for synthesizing the organic polymer precursor, and adding a gelling agent to adjust the pH value of the obtained mixture to 1-2;
(3) stirring the mixture to obtain stable sol in which a carbon source and an aluminum source are uniformly mixed, and cooling to room temperature;
(4) adding a curing agent into the sol at room temperature, stirring to form hydrosol, transferring the hydrosol into a drying oven for drying to obtain dry gel with uniformly mixed carbon source and aluminum source;
(5) grinding and crushing the xerogel, and pyrolyzing the xerogel in a non-oxidizing atmosphere to obtain precursor powder in which aluminum oxide and amorphous carbon are uniformly mixed;
(6) calcining the precursor powder in a flowing atmosphere, and reacting to obtain black powder;
(7) and (3) decarbonizing the black powder in an air atmosphere to obtain the offwhite AlN powder.
2. The method for preparing aluminum nitride nanopowder using sol-gel process according to claim 1, wherein: the aluminum sol in the step (1) is selected from alpha-Al (OH)3Sol, beta-Al (OH)3One or more of sol and AlOOH sol.
3. The method for preparing aluminum nitride nanopowder using sol-gel process according to claim 1, wherein: the gelling agent in the step (2) is selected from nitric acid, hydrochloric acid, acetic acid or ammonia water.
4. The method for preparing aluminum nitride nanopowder using sol-gel process according to claim 1, wherein: the curing agent in the step (4) is one or two of hexamethylenetetramine and polyaldehyde.
5. The method for preparing aluminum nitride nanopowder using sol-gel process according to claim 1, wherein: and (3) drying the oven in the step (4) at the drying temperature of 80-120 ℃.
6. The method for preparing aluminum nitride nanopowder using sol-gel process according to claim 1, wherein: the non-oxidizing atmosphere in the step (5) is selected from N2、Ar、N2-H2One of the mixed gases.
7. The method for preparing aluminum nitride nanopowder using sol-gel process according to claim 1, wherein: the flowing atmosphere in the step (6) is selected from NH3、N2At least one of (1).
8. The method for preparing aluminum nitride nanopowder using sol-gel process according to claim 1, wherein: the pyrolysis temperature in the step (5) is 600-800 ℃; the calcining temperature in the step (6) is 1200-1600 ℃; the carbon removal temperature in the step (7) is 600-800 ℃.
9. The method for preparing aluminum nitride nanopowder using sol-gel process according to claim 1, wherein: the particle size of the AlN powder in the step (7) is 30-200 nm.
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| CN113443611B (en) * | 2021-07-23 | 2022-05-03 | 安徽壹石通材料科技股份有限公司 | Preparation method of nitride powder |
| CN114314531A (en) * | 2022-01-04 | 2022-04-12 | 华东理工大学 | Method for preparing nano aluminum nitride powder by sol-gel foaming |
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