CN115028461A - Method for preparing high-thermal-conductivity silicon nitride ceramic substrate through silicon powder tape casting - Google Patents
Method for preparing high-thermal-conductivity silicon nitride ceramic substrate through silicon powder tape casting Download PDFInfo
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Abstract
The invention relates to a method for preparing a high-thermal-conductivity silicon nitride ceramic substrate by silicon powder tape casting, which comprises the following steps: (1) adding silicon powder serving as raw material powder, at least one of magnesium oxide and calcium oxide serving as a sintering aid A, one of rare earth oxides serving as a sintering aid B and at least one of zirconium oxide, titanium oxide and hafnium oxide serving as a sintering aid C into a solvent containing a dispersing agent, and then adding a binder and a plasticizer and mixing to obtain mixed slurry; (2) defoaming the mixed slurry under the vacuum degree of 10-300 Pa for 5-60 minutes, and then, flowing out a raw material belt with the thickness of 50-1000 microns by adopting curtain coating forming equipment; (3) and cutting and laminating the raw material tape to obtain a silicon nitride substrate blank with required thickness, and then carrying out vacuum de-bonding, nitriding treatment and sintering to obtain the high-thermal-conductivity silicon nitride ceramic substrate.
Description
Technical Field
The invention relates to a preparation method of a silicon nitride ceramic substrate material, in particular to a method for preparing a high-thermal-conductivity silicon nitride ceramic substrate by silicon powder tape casting, and belongs to the field of preparation processes and application of ceramics.
Background
The high-thermal-conductivity silicon nitride ceramic substrate is a key thermal management material for ensuring the safe operation of a high-power electronic device. The power electronic device is a core unit for converting and controlling electric energy in power equipment, and the application field covers various fields such as energy, traffic, basic industry and the like. The development of high power, high frequency and integration is the direction of power electronic devices. The power of the device can reach KW level and even more than tens GW. Due to high energy density and serious heating, the working temperature rises continuously, and the working stability and the service life of the device are seriously influenced. The heat dissipation problem has become a key to be solved. Currently, the commonly used substrate materials are aluminum oxide and aluminum nitride. Alumina cannot effectively dissipate heat due to low thermal conductivity; aluminum nitride ceramics have high thermal conductivity, but are poor in mechanical properties, and are prone to cracking caused by thermal shock during use. Silicon nitride ceramics have the advantages of high thermal conductivity and high reliability, and are currently very advantageous candidate materials.
Silicon nitride ceramics are a conventional structural ceramic material. Has the advantages of high strength, high toughness and excellent high-temperature performance, and has a great amount of application in the industrial and civil fields all the time. In recent years, the silicon nitride ceramic has high heat conductivity and good microwave permeability, and is an ideal ceramic substrate material for high-power electronics by combining good mechanical properties and high-temperature properties. However, for efficient heat transfer, the silicon nitride ceramic substrate is typically only 0.32mm thick, and a common method is tape casting combined with gas pressure sintering.
At present, a commercial tape casting process adopts silicon nitride powder as a raw material to prepare a ceramic thick film through tape casting. Then preparing the ceramic substrate by air pressure sintering. However, high-thermal conductivity silicon nitride ceramic substrates require high-quality silicon nitride powder, which is expensive and completely dependent on import. High-quality silicon powder can be produced domestically and has low price. And the silicon powder has low oxygen content, and the silicon nitride ceramic with high thermal conductivity is easily obtained. Therefore, the development of the silicon powder nitridation sintering process based on localization is a scheme with great commercial value and application prospect.
However, the conventional tape casting process combined with the silicon powder nitridation and sintering process has been difficult to prepare silicon nitride ceramic substrates. Firstly, after the nitridation technology is added, the casting film is easy to deform, and color spots can appear on the surface. These distortions are closely related to the stain and slurry formulation. Therefore, the search for the tape casting, nitriding and sintering process suitable for the silicon powder as the raw material becomes the bottleneck problem at present for preparing the high-quality silicon nitride ceramic substrate. The patent of silicon powder tape casting and nitriding sintering is less. Patent CN201610206078.8 proposes a silicon powder tape casting nitridation sintering process, which uses conventional dispersing agent, binder and plasticizer, unlike the present invention, and does not involve sintering deformation and color problems.
Disclosure of Invention
Aiming at the problems of the traditional tape casting process for preparing the silicon nitride ceramic substrate material by taking silicon powder as a raw material, the invention provides a formula and a process for tape casting for adjustment.
On one hand, the invention provides a method for preparing a high-thermal-conductivity silicon nitride ceramic substrate by silicon powder tape casting, which comprises the following steps:
(1) adding silicon powder serving as raw material powder, at least one of magnesium oxide and calcium oxide serving as a sintering aid A, one of rare earth oxides serving as a sintering aid B and at least one of zirconium oxide, titanium oxide and hafnium oxide serving as a sintering aid C into a solvent containing a dispersing agent, and then adding a binder and a plasticizer and mixing to obtain mixed slurry;
(2) defoaming the mixed slurry under the vacuum degree of 10-300 Pa for 5-60 minutes, and then, flowing out a raw material belt with the thickness of 50-1000 microns by adopting curtain coating forming equipment;
(3) and cutting and laminating the raw material tape to obtain a silicon nitride substrate blank with required thickness, and then carrying out vacuum de-bonding, nitriding treatment and sintering to obtain the high-thermal-conductivity silicon nitride ceramic substrate.
Preferably, the solvent is toluene, 1,1, 1-trichloroethane, ethanol, butanone, a mixed solvent 1 of ethanol and butanone, or a mixed solvent 2 consisting of one of toluene, xylene, 1,1, 1-trichloroethane, methanol, acetone and cyclohexanone and one of ethanol and butanone; the mixed solvent 1 of the ethanol and the butanone comprises 66-90 wt% of the butanone and 10-34 wt% of the ethanol, and the sum of the mass contents of the ethanol and the butanone is 100%; preferably, the composition of the mixed solvent 1 or the mixed solvent 2 is a component corresponding to an azeotropic point of the binary solvent.
Preferably, the total mass percentage of the silicon powder, the sintering aid A, B and the C is (80-95%): (20-5%) and the sum of the mass percentages is 100%; preferably, the sintering aid A, the sintering aid B and the sintering aid C comprise the following components in percentage by mass: (20-50%): (40-70%): 10 percent, and the sum of the mass percentages is 100 percent; the particle size range of the silicon powder is 0.5-20 mu m.
Preferably, the total mass of the silicon powder, the sintering aid A, B and C is used as mixed powder, and the binder is a mixture of polyvinyl butyral and polymethyl methacrylate; the addition amount of the binder is 0.5-15 wt% of the mass of the mixed powder; preferably, the mass percentage content of the polyvinyl butyral and the polymethyl methacrylate in the binder is (10-40%): (60-90%) and the sum of the mass percentage is 100%.
Preferably, the total mass of the silicon powder, the sintering aid A, B and C is used as mixed powder, and the dispersing agent is at least one of castor oil phosphate, ascorbic acid and terpineol; the addition amount of the dispersing agent is 0.5-10 wt% of the total mass of the mixed powder.
Preferably, the total mass of the silicon powder, the sintering aid A, B and C is used as mixed powder, and the plasticizer is a mixture of butyl benzyl phthalate and ethylene glycol; the addition amount of the plasticizer is 0.5-15 wt% of the total mass of the mixed powder; preferably, the mass percentage content of butyl benzyl phthalate and glycol in the plasticizer is (40% -80%): (20-60%) and the sum of the mass percentages is 100%.
Preferably, the vacuum degree of the vacuum debonding is 0.1 to 10KPa, the temperature is 400 to 900 ℃, and the time is 2 to 48 hours.
Preferably, the nitriding atmosphere is a nitrogen atmosphere, the temperature is 1300-1450 ℃, and the heat preservation time is 2-48 hours; preferably, the temperature rise rate of the nitriding treatment is 1-10 ℃/min.
Preferably, the sintering mode is pressureless sintering or air pressure sintering; preferably, the sintering atmosphere is a nitrogen atmosphere, the temperature is 1800-1950 ℃, the air pressure is 0.1-10 MPa, and the time is 1-48 hours; more preferably, the temperature rise rate of the sintering is 0.1-5 ℃/min.
In still another aspect, the present invention provides a high thermal conductive silicon nitride ceramic substrate prepared according to the above method.
Has the advantages that:
the preparation method of the silicon nitride ceramic substrate provided by the invention has the following characteristics. Firstly, the domestic silicon powder is adopted as a raw material, the problems of nitriding, sintering deformation and color spots in the process are combined, the slurry property is regulated and controlled by adjusting the formula and the process of the slurry, finally, the deformation in the nitriding and sintering processes is avoided, and the color uniformity is kept.
Compared with the conventional tape casting preparation scheme, the preparation scheme of the silicon nitride ceramic substrate material provided by the invention has the advantages of low cost, no deformation and uniform color. The basic properties of the silicon nitride ceramic substrate material prepared by the invention are as follows: the density is 3.2 to 3.4g/cm 3 Toughness of 6 to 9MPa m 1/2 And above, the bending strength is 600-900 MPa, and the thermal conductivity is 90-100W/mK. The size of the prepared silicon nitride ceramic substrate material is 138mm multiplied by 190mm multiplied by 0.20-2 mm. Surface roughness: ra is less than or equal to 0.3 m; surface warping degree: is less than 0.15.
Detailed Description
The present invention is further illustrated by the following examples, which are to be understood as merely illustrative and not restrictive.
The invention provides a method for preparing a silicon nitride ceramic substrate by taking silicon powder as a raw material through tape casting, nitriding and post-sintering, which is different from the preparation technology of the commonly used silicon nitride ceramic substrate. Because the silicon powder is used as the raw material, the problems of high price and easy limitation of the high-purity silicon nitride powder can be avoided, and the national production is realized. And the oxygen content of the silicon powder is low, and the thermal conductivity is easy to be higher.
The tape casting technology provided by the invention mainly comprises the steps of taking silicon powder and a sintering aid as raw materials, taking ethanol, butanone, ethanol/butanone or a mixed solvent of toluene and 1,1, 1-trichloroethane or toluene, xylene, 1,1, 1-trichloroethane, methanol, acetone, cyclohexanone, ethanol, butanone and ethanol/butanone as a solvent, taking castor oil phosphate, ascorbic acid and terpineol as dispersing agents, taking a mixture of polyvinyl butyral and polymethyl methacrylate as a binder, and obtaining a biscuit through slurry preparation, defoaming and tape casting. The silicon nitride ceramic substrate is obtained after the steps of debonding, nitriding and sintering. In addition, one of toluene, 1,1, 1-trichloroethane, ethanol and butanone, or one of toluene, xylene, 1,1, 1-trichloroethane, methanol, acetone and cyclohexanone, and one of ethanol and butanone form a mixed solvent 2, and the ethanol/butanone mixed solvent 1 can also be used as a solvent. Wherein the composition of the mixed solvent 1 and the mixed solvent 2 is the azeotropic composition thereof.
The following will illustrate the preparation method of the high thermal conductive silicon nitride ceramic substrate material provided by the present invention by embodiments.
And (4) tape casting. Mixing silicon powder and sintering aid, and dispersing in organic solvent. Specifically, silicon powder and the sintering aid system are dispersed in an organic solvent containing a dispersing agent, then a binder and a plasticizer are added for uniform mixing, and casting is carried out after defoaming to obtain a biscuit.
The solvent is ethanol, butanone or a mixed solvent of ethanol and butanone, the mass content of butanone in an ethanol/butanone system is 66-90%, and the mass content of ethanol is 10-34%; or toluene, 1,1, 1-trichloroethane, or a mixed solvent of toluene, xylene, 1,1, 1-trichloroethane, methanol, acetone, cyclohexanone, ethanol, butanone and ethanol/butanone can be used as the solvent, wherein the composition of the mixed solvent is the azeotropic composition. The dispersing agent is at least one of castor oil phosphate, ascorbic acid and terpineol, and the adding amount of the dispersing agent is 0.5-6 wt% of the total mass of the silicon powder and the sintering aid system. The binder is polyvinyl butyral or polymethyl methacrylate, and the addition amount of the binder is 0.5-10 wt% of the total mass of the mixed powder; wherein the mass percentage of the polyvinyl butyral and the polymethyl methacrylate is (10-40): (60-90). The biscuit also comprises a plastic agent. The plasticizer is a mixture of butyl benzyl phthalate and ethylene glycol, wherein the mass percentage of the butyl benzyl phthalate and the ethylene glycol is (40-80): (20-60). Wherein the particle size of the silicon powder is between 0.5 and 20 mu m. The lamination process is to laminate the single cast films to form a thicker film. The silicon powder is more active and is easy to react with other additives, and particularly when the other additives contain water, the reaction is more serious. Therefore, the formulation of silicon powder casting, the selected dispersing agent, binder and plasticizer will be more careful. The usual dispersants are less suitable; in addition, the effect of PVB which is used as a binder alone is not good; the plasticizers are usually used as binary mixtures. These are all formulations specific to silicon powder casting.
Vacuum de-bonding, nitriding and sintering. The cast film is firstly debonded, and the debonding temperature is usually 400-900 ℃. Nitriding after the de-bonding is finished, wherein the nitriding temperature is in the temperature range of 1300-1450 ℃, the heating rate is 1-10 ℃/min, and the heat preservation time is 2-48 hours; sintering is carried out by adopting pressureless sintering and air pressure sintering processes. The sintering temperature of the silicon nitride ceramic substrate material is 1800-1950 ℃, the air pressure is 0.1-10 MPa, the sintering time is 1-48 h, and the atmosphere is nitrogen atmosphere. The temperature rise rate of the sintering is 0.1-5 ℃/min.
The silicon powder tape casting method is adopted to prepare the silicon nitride ceramic substrate material, and the silicon nitride ceramic substrate material has the same substrate performance as the traditional silicon nitride tape casting process. And has the advantages of low cost and higher heat conductivity, and is a more advantageous preparation scheme of ceramic substrate materials.
The relative density of the silicon nitride ceramic substrate material is measured to be 98-99.5% by adopting an Archimedes drainage method. The thermal conductivity of the silicon nitride ceramic substrate material is measured by adopting a laser thermal conductivity meter method to be 90-100W/mK. MiningMeasuring the toughness of the silicon nitride ceramic substrate material by using a single-side notched beam method to be 6-9 MPa-m 1/2 And the above. And the bending strength of the silicon nitride ceramic substrate material is 600-900 MPa measured by a three-point bending method. Measuring the surface roughness of the silicon nitride ceramic substrate material by using a surface roughness measuring instrument: ra is less than or equal to 0.3 mu m. And measuring the surface warping degree of the silicon nitride ceramic substrate material by adopting a warping degree tester: is less than 0.15 percent.
The present invention will be described in detail by way of examples. It is also to be understood that the following examples are illustrative of the present invention and are not to be construed as limiting the scope of the invention, and that certain insubstantial modifications and adaptations of the invention by those skilled in the art may be made in light of the above teachings. The specific process parameters and the like of the following examples are also only one example of suitable ranges, i.e., those skilled in the art can select the appropriate ranges through the description herein, and are not limited to the specific values exemplified below. Unless otherwise specified, the particle diameters of the silicon nitride powder and the silicon powder in the following examples are generally 0.5 to 20 μm. The particle size distribution of the sintering aid system is 0.5-10 mu m.
Example 1
80g of silicon powder and 20g of sintering aid (6g of magnesium oxide, 12g of yttrium oxide, 2g of zirconium oxide) were added in 50g of ethanol/butanone solvent system (ethanol to butanone mass ratio 34: 66). 3.6g of castor oil phosphate ester is used as a dispersing agent (3.6 wt%), 12g of a binding agent (1.3g of polyvinyl butyral and 10.7 g of polymethyl methacrylate) (12 wt%), 12g of a plastic agent (4.8g of butyl benzyl phthalate and 7.2g of ethylene glycol) (12 wt%), defoaming is carried out for 30min under the vacuum of 100-300mbar after ball milling, and then the ceramic raw material belt is prepared by tape casting. The height of the scraper is 600 microns, and the running speed is 10 cm/min. After drying, the film was cut into a 140mm X140 mm cast film. Then putting the mixture into a vacuum debonding furnace for 2 hours at 900 ℃ for glue discharging, wherein the heating rate is 1 ℃/minute. After the debonding, the sample was placed in a nitrogen/hydrogen gas mixture (N) 2 ：H 2 90:10), keeping the temperature for 48h at 1380 ℃, and increasing the temperature at 5 ℃/min. After nitriding, the casting film is further heated to 1850 ℃ and sintered under the air pressure of 1MPa, and during sinteringAnd cooling the silicon nitride ceramic substrate along with the furnace after 12 hours, and preparing the flat and compact silicon nitride ceramic substrate with uniform color.
Example 2
80g of silicon powder and 20g of sintering aid (6g of magnesium oxide, 12g of yttrium oxide, 2g of zirconium oxide) were added in 50g of ethanol/butanone solvent system (ethanol to butanone mass ratio 34: 66). 3.6g of castor oil phosphate is adopted as a dispersing agent (3.6 wt%), 12g of a binding agent (2.4g of polyvinyl butyral and 9.6g of polymethyl methacrylate) (12 wt%), 12g of a plasticizer (6g of butyl benzyl phthalate and 6g of glycol) (12 wt%), and the raw ceramic tape is prepared by defoaming for 30min under the vacuum of 100-300mbar after ball milling and then tape casting. The height of the scraper is 600 microns, and the running speed is 10 cm/min. After drying, the film was cut into a 140mm X140 mm cast film. Then putting the mixture into a vacuum debonding furnace for glue discharging for 2 hours at 700 ℃, and the heating rate is 1 ℃/minute. After the de-bonding, the sample is nitridized in flowing nitrogen, the nitriding temperature is 1380 ℃, the temperature is kept for 48 hours, and the heating rate is 4 ℃/min. And after nitriding, further heating the casting film to 1880 ℃, sintering at the air pressure of 1MPa for 24 hours, and cooling along with the furnace after the sintering is finished to prepare the flat silicon nitride ceramic substrate with uniform and compact color.
Example 3
80g of silicon powder and 20g of sintering aid (6g of magnesium oxide, 12g of yttrium oxide, 2g of hafnium oxide) were added to a 50g ethanol/butanone solvent system (ethanol to butanone mass ratio 34: 66). 3.6g of ascorbic acid is used as a dispersing agent (3.6 wt%), 12g of a binding agent (3.6g of polyvinyl butyral and 8.4g of polymethyl methacrylate) (12 wt%), 12g of a plastic agent (7.2g of butyl benzyl phthalate and 4.8g of ethylene glycol) (12 wt%), defoaming is carried out for 30min under the vacuum of 100-300mbar after ball milling, and then the ceramic green tape is prepared by tape casting. The height of the scraper is 700 micrometers, and the running speed is 10 cm/min. After drying, the film was cut into a 140mm X140 mm cast film. Then the mixture is put into a vacuum debonding furnace for glue removal for 2 hours at the temperature of 500 ℃ and the heating rate is 1 ℃/minute. After the debonding, the sample was placed in a nitrogen/hydrogen gas mixture (N) 2 ：H 2 90:10), keeping the temperature for 48h at 1400 ℃, and increasing the temperature rate by 3 ℃/min. After nitriding, the casting film is further heated to 1850 ℃, sintered under the pressure of 1MPa for 24 hours, and cooled along with the furnace after the sintering is finished, so as to prepare the flat and color-keeping filmA silicon nitride ceramic substrate with uniform and compact color.
Example 4
80g of silicon powder and 14.2g of sintering aid (4.2g of magnesium oxide, 8.5g of yttrium oxide, 1.5g of hafnium oxide) were added to a 50g ethanol/butanone solvent system (ethanol to butanone mass ratio of 34: 66). 5.4g of ascorbic acid is used as a dispersing agent (5.7 wt%), 14g of a binder (4.2g of polyvinyl butyral and 9.8 g of polymethyl methacrylate) (14.9 wt%), 14g of a plasticizer (8.4g of butyl benzyl phthalate and 5.6g of ethylene glycol) (14.9 wt%), and after ball milling, defoaming is carried out for 30min under the vacuum of 100-300mbar, and then the ceramic green tape is prepared by tape casting. The height of the scraper is 700 micrometers, and the running speed is 10 cm/min. After drying, the film was cut into a 140mm X140 mm cast film. Then the mixture is put into a vacuum debonding furnace to remove glue for 2 hours at 800 ℃, and the heating rate is 1 ℃/minute. After the debonding, the sample was placed in a nitrogen/hydrogen gas mixture (N) 2 ：H 2 90:10), keeping the temperature for 48h at 1380 ℃, and raising the temperature at 5 ℃/min. And after nitriding, further heating the casting film to 1920 ℃, sintering at the air pressure of 5MPa for 36h, and cooling along with the furnace after the sintering is finished to prepare the smooth silicon nitride ceramic substrate with uniform and compact color.
Example 5
80g of silicon powder and 9g of sintering aid (2.7g of calcium oxide, 5.3g of yttrium oxide, 1g of titanium oxide) were added to a 50g ethanol/butanone solvent system (ethanol to butanone mass ratio 34: 66). 3.6g of terpineol is adopted as a dispersing agent (4 wt%), 12g of a binding agent (4.8g of polyvinyl butyral and 7.2g of polymethyl methacrylate) (13.5 wt%), 12g of a plastic agent (8.4g of butyl benzyl phthalate and 3.6g of ethylene glycol) (13.5 wt%), defoaming is carried out for 30min under the vacuum of 100-300mbar after ball milling, and then the ceramic green tape is prepared by tape casting. The height of the scraper is 800 microns, and the running speed is 10 cm/min. After drying, the film was cut into a 200mm X200 mm cast film. Then putting the mixture into a vacuum debonding furnace for 2 hours at 900 ℃ for glue discharging, wherein the heating rate is 1 ℃/minute. After the debonding, the sample was placed in a nitrogen/hydrogen gas mixture (N) 2 ：H 2 90:10), keeping the temperature for 48h at 1450 ℃, and raising the temperature at the rate of 5 ℃/min. After nitriding, the casting film is further heated to 1930 ℃, sintered at the air pressure of 5MPa for 36 hours, and cooled along with the furnace after the sintering is finished, and the prepared flat film is smoothAnd a silicon nitride ceramic substrate with uniform and compact color.
Example 6
80g of silicon powder and 9g of sintering aid (2.7g of calcium oxide, 5.3g of yttrium oxide, 1g of titanium oxide) were added to a 50g ethanol/butanone solvent system (ethanol to butanone mass ratio 34: 66). 7.2g of terpineol is used as a dispersing agent (8.1 wt%), 12g of a binding agent (4.8g of polyvinyl butyral and 7.2g of polymethyl methacrylate) (13.5 wt%), 13.4g of a plastic agent (8.4g of butyl benzyl phthalate and 3.6g of ethylene glycol) (13.5 wt%) is defoamed for 30min under the vacuum of 100-300mbar after ball milling, and then the ceramic green tape is prepared by tape casting. The height of the scraper is 800 microns, and the running speed is 10 cm/min. After drying, the film was cut into a 200mm X200 mm cast film. Then putting the mixture into a vacuum debonding furnace for 2 hours at 900 ℃ for glue discharging, wherein the heating rate is 1 ℃/minute. After the debonding, the sample was placed in a nitrogen/hydrogen gas mixture (N) 2 ：H 2 90:10), keeping the temperature for 48h at 1450 ℃, and raising the temperature at the rate of 5 ℃/min. After nitriding, the casting film is further heated to 1930 ℃, sintered at the air pressure of 5MPa for 36h, and then cooled along with the furnace after the sintering, so that the flat silicon nitride ceramic substrate with uniform and compact color is prepared.
Example 7
80g of silicon powder and 4.3g of sintering aid (1.5g of calcium oxide, 2.5g of yttrium oxide, 0.5g of titanium oxide) were added to a 50g ethanol/butanone solvent system (ethanol to butanone mass ratio 34: 66). 4.8g of terpineol is used as a dispersing agent (5.7 wt%), 12g of a binding agent (4.8g of polyvinyl butyral and 7.2g of polymethyl methacrylate) (14.2 wt%), 12g of a plastic agent (9.6g of butyl benzyl phthalate and 2.4g of ethylene glycol) (14.2 wt%) is defoamed for 30min under the vacuum of 100-300mbar after ball milling, and then the ceramic green tape is prepared by tape casting. The height of the scraper is 800 micrometers, and the running speed is 10 cm/min. After drying, the film was cut into a 140mm X140 mm cast film. Then putting the mixture into a vacuum debonding furnace for 2 hours at 900 ℃ for glue discharging, wherein the heating rate is 1 ℃/minute. After the debonding, the sample was placed in a nitrogen/hydrogen gas mixture (N) 2 ：H 2 90:10), keeping the temperature at 1380 ℃ for 48h, and increasingThe temperature rate was 5 deg.C/min. And after nitriding, further heating the casting film to 1950 ℃, sintering at the air pressure of 10MPa for 48 hours, and cooling along with the furnace after the sintering is finished to prepare the flat silicon nitride ceramic substrate with uniform and compact color.
Example 8
80g of silicon powder and 4.3g of sintering aid (1.5g of calcium oxide, 2.5g of yttrium oxide, 0.5g of titanium oxide) were added to a 50g ethanol/butanone solvent system (ethanol to butanone mass ratio 34: 66). 4.8g of terpineol is used as a dispersing agent (5.7 wt%), 12g of a binding agent (4.8g of polyvinyl butyral and 7.2g of polymethyl methacrylate) (14.2 wt%), 12g of a plastic agent (15.9g of butyl benzyl phthalate and 4.0g of ethylene glycol) (14.2 wt%) is defoamed for 30min under the vacuum of 100-300mbar after ball milling, and then the ceramic green tape is prepared by tape casting. The height of the scraper is 800 microns, and the running speed is 10 cm/min. After drying, the film was cut into a 200mm X200 mm cast film. Then putting the mixture into a vacuum debonding furnace for 2 hours at 900 ℃ for glue discharging, wherein the heating rate is 1 ℃/minute. After the debonding, the sample was placed in a nitrogen/hydrogen gas mixture (N) 2 ：H 2 90:10), keeping the temperature at 1380 ℃ for 48h, and raising the temperature at 5 ℃/min. After nitridation, the casting film is further heated to 1950 ℃, sintered at the air pressure of 10MPa for 48h, and then cooled in a furnace after the sintering is finished, so that the flat, uniform and compact silicon nitride ceramic substrate is prepared, and compared with example 7, the increase of the biscuit size has a certain influence on the warping degree of the sample, but the requirement is still met.
Comparative example 1
80g of silicon powder and 20g of sintering aid (6g of magnesium oxide, 12g of yttrium oxide, 2g of zirconium oxide) were added in 50g of ethanol/butanone solvent system (ethanol to butanone mass ratio 34: 66). 3.6g of castor oil phosphate ester is used as a dispersing agent (3.6 wt%), 12g of a binding agent (1.3g of polyvinyl butyral and 10.7 g of polymethyl methacrylate) (12 wt%), 12g of a plastic agent (4.8g of butyl benzyl phthalate and 7.2g of ethylene glycol) (12 wt%), defoaming is carried out for 30min under the vacuum of 100-300mbar after ball milling, and then the ceramic raw material belt is prepared by tape casting. The height of the scraper is 1200 micrometers, and the running speed is 10 cm/min. After drying, the film was cut into a 140mm by 140mm cast film without lamination. Then the mixture is put into a vacuum debonding furnace for glue discharging for 2 hours at the temperature of 900 ℃, and the heating rate is 1 ℃/minute. DebondingThen the sample is placed in a nitrogen/hydrogen gas mixture (N) 2 ：H 2 90:10), keeping the temperature for 48h at 1380 ℃, and increasing the temperature at 5 ℃/min. And after nitriding, further heating the casting film to 1850 ℃, sintering under the air pressure of 1MPa for 12h, and cooling along with the furnace after the sintering is finished to prepare the compact silicon nitride ceramic substrate with large warping degree and uneven color.
Table 1 shows the performance parameters of the high thermal conductive silicon nitride ceramic substrate materials prepared in examples 1 to 8 and comparative example 1:
Claims (10)
1. a method for preparing a high-thermal-conductivity silicon nitride ceramic substrate by silicon powder tape casting is characterized by comprising the following steps:
(1) adding silicon powder serving as raw material powder, at least one of magnesium oxide and calcium oxide serving as a sintering aid A, one of rare earth oxides serving as a sintering aid B and at least one of zirconium oxide, titanium oxide and hafnium oxide serving as a sintering aid C into a solvent containing a dispersing agent, and then adding a binder and a plasticizer and mixing to obtain mixed slurry;
(2) defoaming the mixed slurry under the vacuum degree of 10-300 Pa for 5-60 minutes, and then, flowing out a raw material belt with the thickness of 50-1000 microns by adopting curtain coating forming equipment;
(3) and cutting and laminating the obtained raw material tape to obtain a silicon nitride substrate blank with the required thickness, and then carrying out vacuum de-bonding, nitriding treatment and sintering to obtain the high-thermal-conductivity silicon nitride ceramic substrate.
2. The method according to claim 1, wherein the solvent is toluene, 1,1, 1-trichloroethane, ethanol, butanone, a mixed solvent 1 of ethanol and butanone, a mixed solvent 2 consisting of one of toluene, xylene, 1,1, 1-trichloroethane, methanol, acetone, cyclohexanone and one of ethanol and butanone; the mixed solvent 1 of the ethanol and the butanone comprises 66-90 wt% of the butanone and 10-34 wt% of the ethanol, and the sum of the mass contents of the ethanol and the butanone is 100%; preferably, the composition of the mixed solvent 1 or the mixed solvent 2 is a component corresponding to an azeotropic point of the binary solvent.
3. The method according to claim 1 or 2, wherein the total mass percentage of the silicon powder and the sintering aid A, B and C is (80-95%): (20-5%) and the sum of the mass percentages is 100%; preferably, the sintering aid A, the sintering aid B and the sintering aid C comprise the following components in percentage by mass: (20-50%): (40-70%): 10 percent, and the sum of the mass percentages is 100 percent; the particle size range of the silicon powder is 0.5-20 mu m.
4. The method according to any one of claims 1 to 3, wherein the total mass of silicon powder, the sintering aid A, B and C is used as mixed powder, and the binder is a mixture of polyvinyl butyral and polymethyl methacrylate; the addition amount of the binder is 0.5-15 wt% of the mass of the mixed powder; preferably, the mass percentage content of the polyvinyl butyral and the polymethyl methacrylate in the binder is (10-40%): (60-90%) and the sum of the mass percentage is 100%.
5. The method according to any one of claims 1 to 4, wherein the total mass of silicon powder, the sintering aid A, B and C is used as mixed powder, and the dispersing agent is at least one of castor oil phosphate, ascorbic acid and terpineol; the addition amount of the dispersing agent is 0.5-10 wt% of the total mass of the mixed powder.
6. The method according to any one of claims 1 to 5, characterized in that the total mass of silicon powder, sintering aid A, B and C is used as mixed powder, the plasticizer is a mixture of butyl benzyl phthalate and glycol; the addition amount of the plasticizer is 0.5-15 wt% of the total mass of the mixed powder; preferably, the mass percentage content of butyl benzyl phthalate and glycol in the plasticizer is (40-80%): (20-60%) and the sum of the mass percentages is 100%.
7. The method according to any one of claims 1 to 6, wherein the vacuum degree of the vacuum debonding is 0.1Pa to 10KPa, the temperature is 500 ℃ to 900 ℃, and the time is 2 hours to 48 hours.
8. The method according to any one of claims 1 to 7, wherein the nitriding atmosphere is a nitrogen atmosphere, the temperature is 1300 to 1450 ℃, and the holding time is 2 to 48 hours; preferably, the temperature rise rate of the nitriding treatment is 1-10 ℃/min.
9. The method according to any one of claims 1 to 8, wherein the sintering is performed by pressureless sintering or gas pressure sintering; preferably, the sintering atmosphere is nitrogen atmosphere, the temperature is 1800-1950 ℃, the air pressure is 0.1-10 MPa, and the time is 1-48 hours; more preferably, the temperature rise rate of the sintering is 0.1-5 ℃/min.
10. A high thermal conductivity silicon nitride ceramic substrate prepared according to the method of any one of claims 1-9.
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