CN108191433B - Modified silicon nitride and preparation method and application of powder containing modified silicon nitride - Google Patents

Modified silicon nitride and preparation method and application of powder containing modified silicon nitride Download PDF

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CN108191433B
CN108191433B CN201711395824.3A CN201711395824A CN108191433B CN 108191433 B CN108191433 B CN 108191433B CN 201711395824 A CN201711395824 A CN 201711395824A CN 108191433 B CN108191433 B CN 108191433B
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李家柱
殷军港
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Yantai University
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Abstract

The invention discloses a modified silicon nitride and a preparation method and application of powder containing the same. The surface grafting modification is carried out by sequentially reacting the hydroxyl on the surface of the silicon nitride powder with the halogenated silane and the hydroxyl-containing organic molecule, thereby obtaining the silicon nitride powder with the surface grafting modification of the organic molecule. The aim is to improve the dispersibility and rheological property of silicon nitride powder water-based slurry for direct solidification injection molding process. Compared with the silicon nitride powder water-based slurry before modification (the solid content is 30-37vol% and 1Pa.s), the solid content of the modified silicon nitride powder water-based slurry obtained by the invention can reach 57-62vol% (1 Pa.s).

Description

Modified silicon nitride and preparation method and application of powder containing modified silicon nitride
Technical Field
The invention relates to a method for grafting and modifying silicon nitride powder by using an organic molecule surface and application thereof, in particular to a method for grafting and modifying silicon nitride powder by using halogenated silane and hydroxyl-containing organic molecules and application thereof.
Background
The preparation of high-performance fine ceramics requires high-quality powder and a mature forming process to guarantee. The colloidal ceramic forming technology is an important ceramic forming method, which can form ceramic parts with various complicated shapes in near net size, and the key point of the technology is to prepare ceramic thick suspension with low viscosity and high solid content, such as Gel Casting (GC) which requires the minimum solid content of 50% (volume fraction, the same below) of ceramic slurry, and direct solidification casting (DCC) which generally requires the solid content of the slurry to be more than 55% and the viscosity of the slurry to be less than 1 Pa.s.
Silicon nitride ceramics become one of the preferred materials for high-temperature structural ceramics due to excellent physical and mechanical properties such as high strength, good thermal shock resistance and oxidation resistance. However, silicon nitride ceramics manufactured by conventional processes have limited applications due to high cost and low reliability. In-situ solidification colloidal forming processes such as DCC and Gel casting have been proposed in recent years as an effective way to solve these problems.
Silicon nitride is a non-oxide powder, which is difficult to disperse in a solvent due to the irregular surface morphology of the powder, complex surface chemical groups (such as amino groups, hydroxyl groups, silane groups and the like) and different specifications and contents of the oxidation sintering agent incorporated in the preparation process, and the dispersion characteristics of different specifications of commercial silicon nitride powder in water are different due to different preparation processes, so that it is difficult to directly prepare a high solid content and low viscosity concentrated suspension. Therefore, the improvement of the dispersibility and rheological property of non-oxide ceramic powder such as silicon nitride in water by a surface modification method is a necessary way to prepare a silicon nitride water-based concentrated suspension with high solid phase volume fraction and low viscosity, and is also a research field which has attracted much attention in recent years. Therefore, the research on the silicon nitride powder surface modification technology has very important scientific and application values, and is also paid more and more attention at present.
In view of the disadvantage that silicon nitride powder is difficult to disperse in water, despite the great progress of the current research, it is still difficult to prepare silicon nitride slurry with solid content higher than 55% suitable for the direct solidification injection molding process, and the effect of the silicon nitride slurry is difficult to make different types of silicon nitride powder meet the practical application requirements.
Disclosure of Invention
In order to solve the problems in the prior art, the invention aims to prepare modified silicon nitride powder by an organic molecule surface grafting method, thereby improving the rheological property and the dispersity of the modified silicon nitride powder in water, obtaining silicon nitride powder water-based slurry with high solid phase content and low viscosity, and preparing high-performance silicon nitride ceramics by a direct solidification injection molding process.
In order to achieve one of the objects of the present invention, a novel silicon nitride compound is provided as follows.
A modified silicon nitride compound represented by the general formula (I):
Figure BDA0001518455280000021
wherein R is selected from-H, -Cl, -Br, -I and-CH3、-CH2CH3、-C6H5；
R' is selected from- (CH)2)nCH3、-CH(CH3)(CH2)nCH3、-CH2C6H5、-(CH2)nOH、
Figure BDA0001518455280000022
Figure BDA0001518455280000023
In the formula, n is 0 or any positive integer.
In order to achieve the second object of the present invention, the following technical means is adopted to provide a method for preparing a powder containing the modified silicon nitride.
The silicon nitride powder is a commercial powder sold in China, the content of alpha-phase is more than 90%, the volume moment average diameter of the particle is 0.7-8 mu m, and the particle shape is irregular.
The technical principle is as follows: the organic molecule surface grafting modification is that silicon hydroxyl on the surface of silicon nitride reacts with halogenated silane and then is grafted with hydroxyl-containing small molecules, so that different organic molecules are grafted on the surface of the silicon nitride in a covalent bond mode.
The preparation method of the powder containing the modified silicon nitride comprises the following steps:
(1) washing with hydrochloric acid: the purpose of this step is to wash away the metal ion impurity complexed with silicon hydroxyl on the surface of the silicon nitride, and improve the concentration of the silicon hydroxyl on the surface, thereby improving the efficiency of grafting modification.
Preparing 20-35 vol% suspension of silicon nitride powder by using 2M hydrochloric acid, transferring the suspension into a ball milling tank, carrying out ball milling or mechanical stirring for 2-8 hours under the conditions that the material ball ratio is 1: 1-2.5 and the rotating speed is 200-.
(2) Washing with deionized water: the purpose of this step is to remove the soluble substances and excess hydrochloric acid formed after the hydrochloric acid washing.
And (2) washing the silicon nitride powder treated in the step (1) by using deionized water, then carrying out centrifugation to accelerate powder precipitation, removing supernatant, and repeating the washing steps until the conductivity value of the supernatant is close to that of the deionized water.
(3) Graft modification: the purpose of the step is to covalently connect organic molecules on the surface of silicon nitride powder by a method of graft modification of halogenated silane and organic molecules containing hydroxyl groups step by step, so as to improve the dispersibility and rheological property of the powder.
Drying the silicon nitride powder washed in the step (2), suspending the silicon nitride powder in anhydrous dichloromethane to prepare 20-40 vol% suspension, adding 0.01-0.2 wt% (the content is the mass percentage of the silicon nitride powder) of halogenated silane, and carrying out ball milling or mechanical stirring for 8-24 hours under the conditions that the material ball ratio is 1: 1-2.5 and the rotating speed is 200-;
then, adding excessive hydroxyl-containing organic molecules, ball-milling or mechanically stirring for 8-24 hours under the conditions that the material ball ratio is 1: 1-2.5 and the rotating speed is 200-.
Preferably, the halosilane is selected from any one of dichlorosilane, trichlorosilane, methyldichlorohydrosilane, ethyldichlorosilane, methyldromohydrosilane, methyldioxohydrogensilane, ethyldibromohydrogensilane, and phenyldichlorohydrogensilane.
Preferably, the hydroxyl-containing organic molecule is selected from any one of methanol, ethanol, n-propanol, isopropanol, n-butanol, isobutanol, sec-butanol, n-pentanol, isopentanol, n-hexanol, n-heptanol, n-octanol, benzyl alcohol, ethylene glycol, 1, 3-propanediol, 1, 4-butanediol, polyethylene glycol, and polyethylene glycol monomethyl ether.
To achieve the third object of the present invention, there is provided a method for producing a modified silicon nitride aqueous slurry using the powder containing a modified silicon nitride compound.
The preparation method of the modified silicon nitride water-based slurry comprises the following steps:
adding modified silicon nitride powder into deionized water, wherein the volume ratio of the modified silicon nitride powder to the water is 1 (0.5-1.5), placing the mixture into a mixing tank, carrying out ball milling or mechanical stirring for 8-24 hours under the conditions that the material ball ratio is 1: 1-2.5 and the rotating speed is 200-500 rpm until the viscosity of the slurry is relatively reduced and stabilized, thus preparing the silicon nitride water-based slurry with the solid phase content of 57-62vol% and the viscosity of not higher than 1Pa.s, wherein the silicon nitride water-based slurry is used for preparing high-performance silicon nitride ceramics.
To achieve the fourth object of the present invention, there is provided use of the modified silicon nitride compound-containing powder.
The modified silicon nitride compound powder is used for preparing high-performance silicon nitride ceramics; preferably, the method is used for preparing the silicon nitride powder water-based slurry with high solid content and low viscosity.
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In order to more clearly illustrate the technical solutions in the embodiments of the present invention, the drawings needed to be used in the embodiments will be briefly described below, and it is obvious that the drawings in the following description are only some embodiments of the present invention, and it is obvious for those skilled in the art that other drawings can be obtained according to these drawings without creative efforts.
FIG. 1 is a schematic diagram of a silicon nitride powder graft-modified with halosilane and hydroxyl-containing organic molecule.
Detailed Description
For better understanding and implementation, the present invention is described in detail below with reference to the following examples, but the scope of the present invention is not limited to these examples, and all changes or equivalent substitutions that do not depart from the spirit of the present invention are included in the scope of the present invention.
In addition, in examples 1 to 9, the added excess hydroxyl-containing organic molecules all refer to hydroxyl-containing organic molecules added in an amount of more than 1% by mass based on the mass of the silicon nitride powder in this example; the preparation method of the modified silicon nitride water-based slurry in the embodiments 1 to 9 is the same as the preparation method of the invention, that is, firstly, the modified silicon nitride powder is added into deionized water, wherein the volume ratio of the modified silicon nitride powder to water is 1 (0.5-1.5), the modified silicon nitride powder is placed in a mixing tank, and after ball milling or mechanical stirring is carried out for 8-24 hours under the conditions that the material ball ratio is 1: 1-2.5 and the rotating speed is 200-.
Example 1:
commercial silicon nitride powder with an alpha-phase content of greater than 90%, particles with a volume moment average diameter of 0.7 μm, a purity of greater than 99%, irregular particle shape, and an initial solids content of 36 vol% (1pa.s) of the aqueous slurry was obtained. The powder modification treatment process comprises the following steps: (1) preparing 30 vol% suspension of silicon nitride powder by using 2M hydrochloric acid, transferring the suspension into a ball milling tank, performing ball milling or mechanical stirring for 8 hours within the range of 200-. (2) Washing the treated silicon nitride powder with deionized water, centrifugally accelerating powder precipitation, removing supernatant, and repeating the steps until the conductivity value of the supernatant is close to that of the deionized water. (3) After being dried, the silicon nitride powder is suspended in anhydrous dichloromethane to prepare 30 vol% suspension, then 0.1 wt% (the content is the percentage of the mass of the silicon nitride powder) of methyl dichlorosilane is added, ball milling or mechanical stirring is carried out for 24 hours within the range of the material ball ratio of 1: 1-2.5 and the rotating speed of 200-500 r/min, after excessive n-hexanol is added, ball milling or mechanical stirring is carried out for 24 hours by the same method, then the solvent is removed, and the silicon nitride powder is washed by water and dried. The water-based slurry prepared from the silicon nitride powder prepared by the method is subjected to ball milling or mechanical stirring for 18 hours, and then the solid content is 62vol% when the apparent viscosity is 1 Pa.s.
Example 2:
commercial silicon nitride powder with an alpha-phase content of greater than 90%, particles with a volume moment average diameter of 0.7 μm, a purity of greater than 99%, irregular particle shape, and an initial solids content of 36 vol% (1pa.s) of the aqueous slurry was obtained. The powder modification treatment process comprises the following steps: (1) preparing 30 vol% suspension of silicon nitride powder by using 2M hydrochloric acid, transferring the suspension into a ball milling tank, performing ball milling or mechanical stirring for 8 hours within the range of 200-. (2) Washing the treated silicon nitride powder with deionized water, centrifugally accelerating powder precipitation, removing supernatant, and repeating the steps until the conductivity value of the supernatant is close to that of the deionized water. (3) After being dried, the silicon nitride powder is suspended in anhydrous dichloromethane to prepare 30 vol% suspension, then 0.05 wt% (the content is the percentage of the mass of the silicon nitride powder) of trichlorosilane is added, ball milling or mechanical stirring is carried out for 12 hours within the range of the material ball ratio of 1: 1-2.5 and the rotating speed of 200-. The water-based slurry prepared from the silicon nitride powder prepared by the method is subjected to ball milling or mechanical stirring for 24 hours, and the solid phase content is 60 vol% when the apparent viscosity is 1 Pa.s.
Example 3:
commercial silicon nitride powder with an alpha-phase content of greater than 90%, particles with a volume moment average diameter of 0.7 μm, a purity of greater than 99%, irregular particle shape, and an initial solids content of 36 vol% (1pa.s) of the aqueous slurry was obtained. The powder modification treatment process comprises the following steps: (1) preparing 30 vol% suspension of silicon nitride powder by using 2M hydrochloric acid, transferring the suspension into a ball milling tank, performing ball milling or mechanical stirring for 8 hours within the range of 200-. (2) Washing the treated silicon nitride powder with deionized water, centrifugally accelerating powder precipitation, removing supernatant, and repeating the steps until the conductivity value of the supernatant is close to that of the deionized water. (3) The silicon nitride powder is dried and then suspended in anhydrous dichloromethane to prepare 25 vol% suspension, then 0.2 wt% (the content is the percentage of the mass of the silicon nitride powder) of dichlorosilane is added, ball milling or mechanical stirring is carried out for 24 hours within the range of the material ball ratio of 1: 1-2.5 and the rotating speed of 200-. The water-based slurry prepared from the silicon nitride powder prepared by the method is subjected to ball milling or mechanical stirring for 18 hours, and then the solid phase content is 59 vol% when the apparent viscosity is 1 Pa.s.
Example 4:
commercial silicon nitride powder with an alpha-phase content of greater than 90%, particles with a volume moment average diameter of 2.3 μm, a purity of greater than 99%, irregular particle shape, and an initial solids content of 33 vol% (1pa.s) of the aqueous slurry was obtained. The powder modification treatment process comprises the following steps: (1) preparing 25 vol% suspension of silicon nitride powder by using 2M hydrochloric acid, transferring the suspension into a ball milling tank, performing ball milling or mechanical stirring for 2 hours within the range of 200-. (2) Washing the treated silicon nitride powder with deionized water, centrifugally accelerating powder precipitation, removing supernatant, and repeating the steps until the conductivity value of the supernatant is close to that of the deionized water. (3) The silicon nitride powder is dried and then suspended in anhydrous dichloromethane to prepare 25 vol% suspension, then 0.1 wt% (the content is the percentage of the mass of the silicon nitride powder) of methyl dichlorosilane is added, ball milling or mechanical stirring is carried out for 24 hours within the range of the material ball ratio of 1: 1-2.5 and the rotating speed of 200 and 500 revolutions per minute, vacuum drying is carried out after the solvent is removed, the silicon nitride powder is suspended in the anhydrous dichloromethane to prepare 25 vol% suspension, excessive n-hexanol is added, ball milling or mechanical stirring is carried out for 24 hours by the same method, then the solvent is removed, water is used for washing and drying are carried out. The water-based slurry prepared from the silicon nitride powder prepared by the method is subjected to ball milling or mechanical stirring for 24 hours, and then the solid phase content is 59 vol% when the apparent viscosity is 1 Pa.s.
Example 5:
commercial silicon nitride powder with an alpha-phase content of greater than 90%, particles with a volume moment average diameter of 2.3 μm, a purity of greater than 99%, irregular particle shape, and an initial solids content of 33 vol% (1pa.s) of the aqueous slurry was obtained. The powder modification treatment process comprises the following steps: (1) preparing 25 vol% suspension of silicon nitride powder by using 2M hydrochloric acid, transferring the suspension into a ball milling tank, performing ball milling or mechanical stirring for 2 hours within the range of 200-. (2) Washing the treated silicon nitride powder with deionized water, centrifugally accelerating powder precipitation, removing supernatant, and repeating the steps until the conductivity value of the supernatant is close to that of the deionized water. (3) After being dried, the silicon nitride powder is suspended in anhydrous dichloromethane to prepare 25 vol% suspension, then 0.01 wt% (the content is the percentage of the mass of the silicon nitride powder) of trichlorosilane is added, ball milling or mechanical stirring is carried out for 24 hours within the range of the material ball ratio of 1: 1-2.5 and the rotating speed of 200-. The water-based slurry prepared from the silicon nitride powder prepared by the method is subjected to ball milling or mechanical stirring for 24 hours, and then the solid phase content is 61 vol% when the apparent viscosity is 1 Pa.s.
Example 6:
commercial silicon nitride powder with an alpha-phase content of greater than 90%, particles with a volume moment average diameter of 2.3 μm, a purity of greater than 99%, irregular particle shape, and an initial solids content of 33 vol% (1pa.s) of the aqueous slurry was obtained. The powder modification treatment process comprises the following steps: (1) preparing 25 vol% suspension of silicon nitride powder by using 2M hydrochloric acid, transferring the suspension into a ball milling tank, performing ball milling or mechanical stirring for 2 hours within the range of 200-. (2) Washing the treated silicon nitride powder with deionized water, centrifugally accelerating powder precipitation, removing supernatant, and repeating the steps until the conductivity value of the supernatant is close to that of the deionized water. (3) The silicon nitride powder is dried and then suspended in anhydrous dichloromethane to prepare 25 vol% suspension, then 0.1 wt% (the content is the percentage of the mass of the silicon nitride powder) of dichlorosilane is added, ball milling or mechanical stirring is carried out for 24 hours within the range of the material ball ratio of 1: 1-2.5 and the rotating speed of 200-. The water-based slurry prepared from the silicon nitride powder prepared by the method is subjected to ball milling or mechanical stirring for 24 hours, and then the solid phase content is 57 vol% when the apparent viscosity is 1 Pa.s.
Example 7:
commercial nanoscale silicon nitride powders having an alpha-phase content of greater than 90%, particles with a volume moment average diameter of 40nm, a purity of greater than 99%, irregular particle shapes, and an initial solids content of 30 vol% (1Pa.s) in the aqueous slurry are commercially available. The powder modification treatment process comprises the following steps: (1) preparing 20 vol% suspension of silicon nitride powder by using 2M hydrochloric acid, transferring the suspension into a ball milling tank, performing ball milling or mechanical stirring for 6 hours within the range of 200-. (2) Washing the treated silicon nitride powder with deionized water, centrifugally accelerating powder precipitation, removing supernatant, and repeating the steps until the conductivity value of the supernatant is close to that of the deionized water. (3) The silicon nitride powder is dried and then suspended in anhydrous dichloromethane to prepare 25 vol% suspension, then 0.1 wt% (the content is the percentage of the mass of the silicon nitride powder) of methyl dichlorosilane is added, ball milling or mechanical stirring is carried out for 24 hours within the range of the material ball ratio of 1: 1-2.5 and the rotating speed of 200 and 500 revolutions per minute, vacuum drying is carried out after the solvent is removed, the silicon nitride powder is suspended in the anhydrous dichloromethane to prepare 25 vol% suspension, excessive n-hexanol is added, ball milling or mechanical stirring is carried out for 24 hours by the same method, then the solvent is removed, water is used for washing and drying are carried out. The water-based slurry prepared from the silicon nitride powder prepared by the method is subjected to ball milling or mechanical stirring for 24 hours, and then the solid phase content is 57 vol% when the apparent viscosity is 1 Pa.s.
Example 8:
commercial nanoscale silicon nitride powders having an alpha-phase content of greater than 90%, particles with a volume moment average diameter of 40nm, a purity of greater than 99%, irregular particle shapes, and an initial solids content of 30 vol% (1Pa.s) in the aqueous slurry are commercially available. The powder modification treatment process comprises the following steps: (1) preparing 20 vol% suspension of silicon nitride powder by using 2M hydrochloric acid, transferring the suspension into a ball milling tank, performing ball milling or mechanical stirring for 2 hours within the range of 200-. (2) Washing the treated silicon nitride powder with deionized water, centrifugally accelerating powder precipitation, removing supernatant, and repeating the steps until the conductivity value of the supernatant is close to that of the deionized water. (3) After being dried, the silicon nitride powder is suspended in anhydrous dichloromethane to prepare 25 vol% suspension, then 0.05 wt% (the content is the percentage of the mass of the silicon nitride powder) of trichlorosilane is added, ball milling or mechanical stirring is carried out for 24 hours within the range of the material ball ratio of 1: 1-2.5 and the rotating speed of 200-. The water-based slurry prepared from the silicon nitride powder prepared by the method is subjected to ball milling or mechanical stirring for 24 hours, and the solid phase content is 58 vol% when the apparent viscosity is 1 Pa.s.
Example 9:
commercial nanoscale silicon nitride powders having an alpha-phase content of greater than 90%, particles with a volume moment average diameter of 40nm, a purity of greater than 99%, irregular particle shapes, and an initial solids content of 30 vol% (1Pa.s) in the aqueous slurry are commercially available. The powder modification treatment process comprises the following steps: (1) preparing 20 vol% suspension of silicon nitride powder by using 2M hydrochloric acid, transferring the suspension into a ball milling tank, performing ball milling or mechanical stirring for 2 hours within the range of 200-. (2) Washing the treated silicon nitride powder with deionized water, centrifugally accelerating powder precipitation, removing supernatant, and repeating the steps until the conductivity value of the supernatant is close to that of the deionized water. (3) The silicon nitride powder is dried and then suspended in anhydrous dichloromethane to prepare 25 vol% suspension, then 0.05 wt% (the content is the percentage of the mass of the silicon nitride powder) of dichlorosilane is added, ball milling or mechanical stirring is carried out for 24 hours within the range of the material ball ratio of 1: 1-2.5 and the rotating speed of 200-. The water-based slurry prepared from the silicon nitride powder prepared by the method is subjected to ball milling or mechanical stirring for 24 hours, and then the solid phase content is 57 vol% when the apparent viscosity is 1 Pa.s.

Claims (4)

1. A modified silicon nitride compound represented by the general formula (I),
Figure DEST_PATH_IMAGE002
wherein R is selected from-H, -Cl, -Br, -I and-CH3、-CH2CH3、-C6H5；
R' is selected from- (CH)2)nCH3、-CH(CH3)(CH2)nCH3、-CH2C6H5、-(CH2)nOH、
Figure DEST_PATH_IMAGE004
Figure DEST_PATH_IMAGE006
n is 0 or any positive integer.
2. A method for preparing powder containing the modified silicon nitride compound of claim 1, comprising the steps of using silicon nitride powder having an alpha-phase content of more than 90%, a volume moment average diameter of particles of 0.7 μm to 40nm, and a purity of more than 99%,
(1) washing with hydrochloric acid:
preparing a suspension with the silicon nitride powder concentration of 20-35 vol% by using 2M hydrochloric acid, transferring the suspension into a ball milling tank, carrying out ball milling for 2-8 hours under the conditions that the material-ball ratio is 1 (1-2.5) and the rotating speed is 200-;
(2) washing with deionized water:
washing the silicon nitride powder treated in the step (1) with deionized water, then centrifuging to accelerate the precipitation of the silicon nitride powder and removing supernatant, and repeating the washing step until the conductivity value of the supernatant is close to that of the deionized water;
(3) graft modification:
drying the silicon nitride powder washed in the step (2), suspending the dried silicon nitride powder in anhydrous dichloromethane to prepare a suspension with the silicon nitride powder concentration of 20-40 vol%, adding halosilane with the mass of 0.01-0.2 wt% of the silicon nitride powder, and performing ball milling for 8-24 hours under the conditions that the ball-feed ratio is 1 (1-2.5) and the rotating speed is 200-;
then adding hydroxyl-containing organic molecules with the mass more than 1 percent of that of the silicon nitride powder, ball-milling or mechanically stirring for 8-24 hours under the conditions that the material-ball ratio is 1 (1-2.5) and the rotating speed is 200-500 r/m, then removing the anhydrous dichloromethane solvent, washing with water and drying to obtain the powder containing the modified silicon nitride compound in the claim 1;
the halogenated silane is selected from any one of dichlorosilane, trichlorosilane, methyl dichlorosilane, ethyl dichlorosilane, methyl dibromosilane, methyl diiodohydrosilane, ethyl dibromosilane and phenyl dichlorosilane;
the hydroxyl-containing organic molecule is selected from any one of methanol, ethanol, n-propanol, isopropanol, n-butanol, isobutanol, sec-butanol, n-pentanol, isoamyl alcohol, n-hexanol, n-heptanol, n-octanol, benzyl alcohol, ethylene glycol, propylene glycol, butanediol, polyethylene glycol and polyethylene glycol monomethyl ether.
3. A method for preparing modified silicon nitride water-based slurry by using the powder containing the modified silicon nitride compound obtained by the preparation method of claim 2 is characterized in that the powder containing the modified silicon nitride compound is added into deionized water and placed in a mixing tank, wherein the volume ratio of the powder containing the modified silicon nitride compound to water is 1 (0.5-1.5), and ball milling or mechanical stirring is carried out for 8-24 hours under the conditions that the ball-to-ball ratio is 1 (1-2.5) and the rotating speed is 200-500 rpm until the viscosity of the slurry is relatively reduced and stabilized, so that the modified silicon nitride water-based slurry with the solid phase content of 57-62vol% and the viscosity of not higher than 1Pa.s is prepared.
4. Use of the modified silicon nitride compound-containing powder produced by the production method according to claim 2, characterized in that the modified silicon nitride compound-containing powder is used for producing a silicon nitride powder aqueous slurry having a solid content of 57 to 62vol% and a viscosity of not higher than 1 pa.s.
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