CN114890797A - Preparation method of silicon nitride ceramic substrate - Google Patents
Preparation method of silicon nitride ceramic substrate Download PDFInfo
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- CN114890797A CN114890797A CN202210437896.4A CN202210437896A CN114890797A CN 114890797 A CN114890797 A CN 114890797A CN 202210437896 A CN202210437896 A CN 202210437896A CN 114890797 A CN114890797 A CN 114890797A
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Abstract
The invention relates to a preparation method of a silicon nitride ceramic substrate, which comprises the following steps: (1) adding at least one of silicon nitride powder, silicon powder and sintering aid into a solvent containing a dispersing agent, carrying out ball milling and mixing, then adding a binder and a plasticizer, continuing ball milling and mixing, and carrying out vacuum defoaming to obtain mixed slurry; the adhesive is polypropylene carbonate, and the addition amount of the adhesive is 1-20 wt% of the total mass of the raw material powder and the sintering aid; (2) preparing the obtained mixed slurry into a green ceramic chip by using tape casting equipment; (3) cutting and laminating the plurality of green ceramic chips to obtain a silicon nitride biscuit with required thickness; (4) and performing de-bonding and air pressure sintering on the obtained silicon nitride biscuit to obtain the silicon nitride ceramic substrate.
Description
Technical Field
The invention relates to a preparation method of a silicon nitride ceramic substrate, belonging to the field of preparation process and application of ceramics.
Background
The development trend of high integration and microminiaturization of electronic devices leads to higher and higher power and gradual rise of the working temperature of the devices, and once the safe working temperature of a chip is exceeded, the thermal failure and stress damage of the chip can be caused, so that the service life of the electronic devices is shortened. In order to transmit the heat generated by the device in time, a substrate material with a good heat dissipation effect needs to be selected.
Common substrate materials for ceramics are aluminum oxide, beryllium oxide, and aluminum nitride. The alumina ceramic is widely applied with the advantages of low cost and mature process, but the thermal conductivity and the mechanical property of the alumina ceramic are not high, and the requirements of heat dissipation and device reliability cannot be met; the beryllium oxide ceramic has high thermal conductivity and can effectively dissipate heat, but the raw materials of the beryllium oxide ceramic have toxicity and cannot be widely applied in industry; the thermal conductivity of the aluminum nitride ceramic is as high as 170-240W/(m.K), the aluminum nitride ceramic has outstanding advantages in the aspect of heat dissipation, but the aluminum nitride ceramic has poor mechanical properties, is easy to crack due to thermal shock, and has limited application prospects. Silicon nitride ceramic is a structural ceramic with high heat and high mechanical property, the thermal conductivity of the silicon nitride ceramic is superior to that of alumina ceramic, and the mechanical property of the silicon nitride ceramic is superior to that of the alumina ceramic and the aluminum nitride ceramic, so the silicon nitride ceramic is an ideal heat-radiating substrate substitute material.
The silicon nitride ceramic substrate forming method mainly comprises two methods: one is dry pressing, the silicon nitride ceramic substrate prepared by the method is thick, and needs to be further cut into a substrate with required thickness, so that the cost is increased; the other is tape casting, the thickness is easy to control, and the tape casting is suitable for large-scale production and has lower cost. Compared with dry pressing molding, tape casting molding has more superiority.
The silicon nitride tape casting process is relatively mature, and an organic tape casting system is generally adopted. The tape-casting process uses Polyvinyl Butyral (PVB) as a binder, and the binder has more residual carbon after cracking and influences the performance of the final material.
Disclosure of Invention
Aiming at the problems of the traditional tape casting process for preparing the silicon nitride ceramic substrate material by taking PVB as a binder, the formula and the process of the tape casting are adjusted, and the preparation method of the silicon nitride ceramic substrate is further provided, which comprises the following steps:
(1) adding at least one of silicon nitride powder, silicon powder and sintering aid into a solvent containing a dispersing agent, carrying out ball milling and mixing, then adding a binder and a plasticizer, continuing ball milling and mixing, and carrying out vacuum defoaming to obtain mixed slurry; the binder is polypropylene carbonate, and the addition amount of the binder is 1-20 wt% (preferably 1-15 wt%) of the total mass of the raw material powder and the sintering aid;
(2) preparing the obtained mixed slurry into a green ceramic chip by using tape casting equipment;
(3) cutting and laminating the plurality of green ceramic chips to obtain a silicon nitride biscuit with required thickness;
(4) and carrying out de-bonding and air pressure sintering on the obtained silicon nitride biscuit to obtain the silicon nitride ceramic substrate.
The invention focuses on applying PPC to silicon nitride tape casting to obtain a high-quality tape casting film through regulation and control. Experiments prove that the PPC is used as a binder, a casting film with low carbon content and no defects can be obtained, and the prepared ceramic also has high thermal conductivity and excellent bending strength.
Preferably, the sintering aid is selected from MgO and Y 2 O 3 Or at least one of rare earth oxides; wherein the mass ratio of the raw material powder to the sintering aid is (75-97): (25-3), wherein the sum of the mass percentages of the two is 100 wt%. The rare earth oxide in the sintering aid accounts for 5-20 wt% of the total mass of the raw material powder and the sintering aid.
Preferably, the solvent is ethyl acetate, butanone or a mixed solvent of ethyl acetate and butanone; when the solvent is a mixed solvent of ethyl acetate and butanone, the mass content of the butanone is 70-90 wt%, the mass content of the ethyl acetate is 10-30 wt%, and the sum of the mass percentages of the ethyl acetate and the ethyl acetate is 100 wt%; the mass of the solvent is 30-60 wt% of the total mass of the raw material powder and the sintering aid. When the raw material powder is silicon nitride powder, the preferred weight percentage of the solvent is 40-50 wt% of the total weight of the raw material powder and the sintering aid; when the raw material powder is silicon powder, the mass of the solvent is preferably 35-45 wt% of the total mass of the raw material powder and the sintering aid. If the solvent is too much, the slurry is thin, the powder content of the casting film is low, the shrinkage is large, the density and the flatness of the substrate are low, and the thermal conductivity and the bending strength of the substrate are affected. If the solvent is too little, the slurry is too thick, powder particles in the casting film are not uniformly distributed, and the agglomeration phenomenon exists, so that more defects are caused, the structure of the substrate is influenced, and the heat conductivity and the bending strength of the substrate are further hindered.
Preferably, the particle size range of the silicon nitride powder is 0.1-10 μm, the particle size range of the silicon powder is 0.1-10 μm, and the particle size range of the sintering aid is 0.1-10 μm.
Preferably, the dispersant is at least one of castor oil, triolein and phosphate, and the addition amount of the dispersant is 0.5-10% of the total mass of the raw material powder and the sintering aid.
Preferably, the plasticizer is a mixture of butyl benzyl phthalate and polyethylene glycol-400, the total content of the plasticizer is 0.1-5 times of the binder content, and is 1-5 wt% of the total mass of the raw material powder and the sintering aid, wherein the mass ratio of butyl benzyl phthalate to polyethylene glycol-400 is 0.1-5.
Preferably, the rotation speed of the ball milling mixing is 10-500 r/min, and the total ball milling time is 48-144 hours. The vacuum degree of the vacuum defoaming is less than or equal to 220mbar, the stirring speed is 10-50 r/min, and the defoaming time is 10-50 minutes
Preferably, when the raw material powder is silicon nitride powder, the addition amount of the binder is 12-17 wt% of the total mass of the raw material powder and the sintering aid, and is preferably 13.5 wt%; when the raw material powder is silicon powder, the addition amount of the binder is 12-15 wt%, preferably 13wt% of the total mass of the raw material powder and the sintering aid. If the binder is too much, the slurry is too thick, the defects of the casting film and the contained organic matters are more, the powder content is correspondingly lower, the sintering of ceramics is not facilitated, the density of the substrate is reduced, and the thermal conductivity and the bending strength of the substrate are influenced; if the binder is too little, the strength of the casting film is low, the casting film is not easy to store and sample, the density, the flatness and the uniformity of the substrate can be correspondingly influenced, and the thermal property and the mechanical property of the substrate are further influenced.
Preferably, in the tape casting process, the height of the scraper is 10-100 mm, and the tape casting speed is 50-150 mm/min. Preferably, the thickness of the green ceramic chip is 5-40 mm.
Preferably, the debonding atmosphere is vacuum, the temperature is 400-600 ℃, and the heat preservation time is 1-24 hours; preferably, the temperature rise rate of the de-bonding is 1-10 ℃/min.
Preferably, when the raw material powder contains silicon powder, after the debinding and before the air pressure sintering, the debinded silicon nitride biscuit is subjected to nitriding treatment for 2-48 hours at 1200-1500 ℃ in a nitrogen atmosphere; preferably, the temperature rise rate of the nitriding treatment is 1-10 ℃/min.
Preferably, the parameters of the gas pressure sintering comprise; the sintering atmosphere is nitrogen, the temperature is 1700-1900 ℃, the heat preservation time is 1-24 hours, and the air pressure is 0.1-10 MPa; preferably, the temperature rise rate and the temperature drop rate of the air pressure sintering are respectively 1-5 ℃/min.
In another aspect, the present invention provides a silicon nitride ceramic substrate prepared according to the above preparation method.
Has the advantages that:
the invention adopts a tape casting process, takes at least one of silicon nitride powder and silicon powder as a raw material, takes MgO, CaO and rare earth oxide as a sintering aid system, and prepares a biscuit with a smooth surface and no defects by adding a proper organic solvent, a dispersing agent, a binder and a plasticizer and controlling the content ratio. Then the biscuit is laminated to obtain a biscuit block, and the silicon nitride ceramic substrate material with high thermal conductivity and excellent mechanical property is prepared through reasonable de-bonding, (nitriding) and sintering processes.
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 no deformation and low impurity content. 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 The bending strength is 600-1100 MPa, the thermal conductivity is 50-100W/(m.K), and the free carbon content: is less than 0.15 percent.
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 using PPC as a binder through tape casting, (nitriding) and sintering, which is different from the preparation technology of the commonly used silicon nitride ceramic substrate. Because PPC is adopted as the binder, the content of impurities in the silicon nitride ceramic can be effectively reduced, and the improvement of the performance of the silicon nitride ceramic is facilitated.
Specifically, the polypropylene carbonate (PPC) has the advantages of no residue after decomposition, low carbon residue, safe decomposition in both aerobic and anaerobic environments and the like, and is applied to silicon nitride ceramic tape casting to help reduce impurities in the silicon nitride ceramic and improve the silicon nitride ceramic tape casting. In addition, after the casting film is laminated, the proper de-bonding, nitriding and sintering processes are adopted without layering and warping, so that the method has important significance for large-scale preparation of the silicon nitride ceramic substrate with excellent thermal conductivity and mechanical property. The invention optimizes the casting formula, reduces the content of free carbon, ensures that the surface of the prepared casting film is smooth and has no defects, and the sintered compact ceramic has higher thermal conductivity and bending strength.
The tape casting technology provided by the invention mainly comprises the steps of taking silicon nitride powder/silicon powder and a sintering aid as raw materials, taking ethyl acetate, butanone and ethyl acetate/butanone as solvents, taking castor oil, triolein and phosphate ester as dispersing agents, taking PPC as a binder, taking a mixture of butyl benzyl phthalate and polyethylene glycol-400 as a plasticizer, and obtaining a biscuit through slurry preparation, vacuum defoaming and tape casting. Then the silicon nitride ceramic substrate is obtained through debonding, (nitriding) and sintering. 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 mixing the raw material powder and the sintering aid to obtain mixed powder. Wherein the particle size range of the silicon nitride powder and the silicon powder is 0.1-10 mu m. Magnesium oxide or/and calcium oxide is used as a sintering aid A, one or more rare earth oxides are used as a sintering aid B, and the mass ratio of the sintering aid A to the sintering aid B is 1: (1-10). The mass ratio of the raw material powder to the sintering aid is (75-97): (25-3).
Ball-milling the mixed powder in a solvent containing a dispersing agent, and then adding a binder and a plasticizer for secondary ball-milling to obtain mixed slurry with a uniform structure. The organic solvent is at least one of ethyl acetate and butanone, and the mass of the solvent accounts for 10-50% of the total mass of the mixed powder of the raw material powder and the sintering aid. The dispersant is at least one of castor oil, triolein and phosphate, and the addition amount of the dispersant is 0.5-10% of the total mass of the mixed powder. The adhesive is PPC, and the addition amount is 1-20% of the total mass of the mixed powder. The plasticizer is a mixture of butyl benzyl phthalate and polyethylene glycol-400, the total content of the plasticizer mixture is 10% -50% of the binder content, and the mass ratio of the butyl benzyl phthalate to the polyethylene glycol-400 is 0.1-10. Aiming at a silicon nitride tape casting system, the PPC adhesive is used to effectively reduce the content of the plasticizer, so that the total content of organic matters in the slurry is reduced, and the ceramic density and performance are improved.
And (3) defoaming the slurry in vacuum, and then carrying out a casting forming process to obtain a casting biscuit (green ceramic chip). The vacuum degree of the vacuum defoaming is 220mbar, the stirring speed is 10-50 r/min, and the defoaming time is 10-50 mins.
And cutting and laminating the casting biscuit, carrying out glue discharging treatment, and carrying out (nitriding) and sintering to obtain the silicon nitride ceramic substrate. The de-bonding process is carried out in vacuum, the de-bonding temperature is 400-600 ℃, the time is 1-24 h, and the heating rate is 1-5 ℃/min. The nitriding temperature is within the range of 1200-1450 ℃, and the nitriding atmosphere is N 2 The time is 2-48 h, and the heating rate is 1-10 ℃/min. The sintering mode is air pressure sintering. The sintering atmosphere is N 2 The temperature is 1700-1900 ℃, the air pressure is 0.1-10 MPa, the time is 1-24 h, and the temperature rise rate is 1-10 ℃/min. The pressure of the lamination is 1-10 MPa, and the pressure maintaining time is 1-10 minutes.
In the invention, the density of the silicon nitride ceramic substrate obtained by adopting an Archimedes drainage method to test is 3.2-3.4 g/cm 3 。
In the invention, the bending strength of the obtained silicon nitride ceramic substrate is 600-1100 MPa by adopting a three-point bending method.
In the invention, the thermal conductivity of the silicon nitride ceramic substrate obtained by adopting a laser thermal conductivity instrument is 50-100W/(m.K).
In the invention, the free carbon content of the obtained silicon nitride ceramic substrate is less than 0.15 percent by adopting a chemical method.
The present invention will be described in further detail with reference to 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.
Example 1
4g of glycerol trioleate as a dispersant was added into a 62.7g ethyl acetate/butanone solvent system (the mass ratio of ethyl acetate to butanone was 78:22, and the weight ratio of ethyl acetate to butanone was 43.1 wt% of the mixed powder), and after sufficient dispersion, 128g of silicon nitride powder and 17.52g of sintering aid (4.38g of magnesium oxide and 13.14g of erbium oxide) were added thereto. After ball milling for 24h, 19.6g of binder PPC (13.5 wt%) and 4.9g of plasticizer (2.45g of butyl benzyl phthalate and 2.45g of polyethylene glycol-400, the ratio R of the plasticizer to the binder is 0.25) are added, after ball milling for 48h, defoaming is carried out in vacuum for 20mins, and then casting is adopted to prepare the casting film. The height of the doctor blade was 40mm and the casting speed was 120 mm/min. After drying, the cast film was cut into a thickness of 50mm X50 mm (thickness: 0.183 mm). And (3) putting 10 cast films into a die with the thickness of 50mm multiplied by 50mm, applying pressure to the cast films by using a manual hydraulic press at 20MPa, maintaining the pressure for 1min, putting the cast films into a 60 ℃ oven, preserving the temperature for 1h, taking the cast films out, applying the same pressure again, and naturally cooling to obtain the silicon nitride biscuit. Then the biscuit is put into a vacuum debonding furnace for vacuum debonding for 2 hours at the temperature of 600 ℃, and the heating rate is 1 ℃/min. After the de-bonding, the sample is sintered at 1830 ℃ in nitrogen with the pressure of 0.3MPa for 2h, and then cooled along with the furnace.
Example 2
The process of the silicon nitride ceramic substrate of example 2 is as described in example 1, except that: the adding amount of the solvent is 45.9 wt% of the total mass of the raw material powder and the sintering aid.
Example 3
The process of the silicon nitride ceramic substrate of example 3 is as described in example 1, except that: the adding amount of the poly propylene carbonate is 11.5 wt% of the total mass of the raw material powder and the sintering aid.
Example 4
The process of the silicon nitride ceramic substrate of example 4 is as described in example 1, except that: the addition amount of the poly (propylene carbonate) is 12.5 wt% of the total mass of the raw material powder and the sintering aid.
Example 5
The process of the silicon nitride ceramic substrate of the present example 5 is referred to example 1, except that: the adding amount of the poly (propylene carbonate) is 14.0 wt% of the total mass of the raw material powder and the sintering aid.
Example 6
4.8g of triolein as a dispersant was added to 60g of an ethyl acetate/butanone solvent system (the mass ratio of ethyl acetate to butanone was 78:22, accounting for 38.33 wt% of the mixed powder), and after sufficient dispersion, 127.55g of silicon powder and 28.99g of a sintering aid (7.24g of magnesium oxide; 21.75g of erbium oxide, accounting for 14 wt% of the total powder) were added thereto. After ball milling, 20.35g of binder PPC (13.0 wt%) and 4g of plasticizer (2g of butyl benzyl phthalate and 2g of polyethylene glycol-400, wherein the ratio R of the plasticizer to the binder is 0.20) are added, after ball milling for 48 hours, defoaming is carried out in vacuum for 20mins, and then casting molding is adopted to prepare the casting film. The height of the doctor blade was 40mm and the casting speed was 120 mm/min. After drying, the film was cut into a 50mm X50 mm cast film (thickness: 0.167 mm). And (3) putting 10 cast films into a die with the thickness of 50mm multiplied by 50mm, applying pressure to the cast films by using a manual hydraulic press at 20MPa, maintaining the pressure for 1min, putting the cast films into a 60 ℃ oven, preserving the temperature for 1h, taking the cast films out, applying the same pressure again, and naturally cooling to obtain the silicon nitride biscuit. Then the biscuit is put into a vacuum debonding furnace for vacuum debonding for 2 hours at the temperature of 600 ℃, and the heating rate is 1 ℃/min. After the debonding, the sample was nitrided at 1420 ℃ in nitrogen and kept for 2 h. Then sintering at 1830 ℃ in nitrogen with the air pressure of 0.3MPa for 2h, and cooling along with the furnace after the sintering.
Example 7
The process for producing the silicon nitride ceramic substrate of example 7 is as described in example 6, except that: the addition amount of the polypropylene carbonate is 11 wt% of the total mass of the raw material powder and the sintering aid.
Example 8
The process for producing the silicon nitride ceramic substrate of example 8 is as described in example 6, except that: the addition amount of the polypropylene carbonate is 12 wt% of the total mass of the raw material powder and the sintering aid.
Example 9
The process for producing the silicon nitride ceramic substrate of example 9 is as described in example 6, except that: the adding amount of erbium oxide is 9 wt% of the total mass of the raw material powder and the sintering aid.
Example 10
The process for producing the silicon nitride ceramic substrate of the present example 10 is as described in example 6, except that: the adding amount of erbium oxide is 17wt% of the total mass of the raw material powder and the sintering aid.
Comparative example 1
Comparative example 1 differs from example 1 only in that: the same applies to comparative example 1, in which the same amount of PVB binder is used instead of PPC, and the description is omitted here.
Comparative example 2
Comparative example 2 differs from example 1 only in that: the adding amount of the poly (propylene carbonate) is 17wt% of the total mass of the raw material powder and the sintering aid.
Comparative example 3
Comparative example 3 differs from example 6 only in that: the erbium oxide sintering aid was replaced by an yttrium oxide sintering aid, the rest of which was the same as in example 1 and will not be described again here.
Table 1 shows the properties of the samples described in the examples and comparative examples:
as can be seen from Table 1, the ceramic prepared by the higher solid content has higher density, thermal conductivity and bending strength, and the increase of the PPC content is beneficial to the improvement of the tensile strength and the breaking strain of the green ceramic chip, but the density is reduced; the PVB-containing samples had lower carbon residue than the PPC samples.
In conclusion, the PPC is adopted as the binder, and the prepared silicon nitride ceramic substrate has good purity and performance, low free carbon content, high thermal conductivity and excellent mechanical property. In the invention, the PPC adhesive is adopted, so that the content of the used plasticizer is correspondingly reduced, thereby reducing the total organic matter content, and being beneficial to improving the density of the biscuit and the performance of the ceramic.
Claims (10)
1. A method for preparing a silicon nitride ceramic substrate, comprising:
(1) adding at least one of silicon nitride powder, silicon powder and sintering aid into a solvent containing a dispersing agent, carrying out ball milling and mixing, then adding a binder and a plasticizer, continuing ball milling and mixing, and carrying out vacuum defoaming to obtain mixed slurry; the adhesive is polypropylene carbonate, and the addition amount of the adhesive is 1-20 wt% of the total mass of the raw material powder and the sintering aid;
(2) preparing the obtained mixed slurry into a green ceramic chip by using tape casting equipment;
(3) cutting and laminating the plurality of green ceramic chips to obtain a silicon nitride biscuit with required thickness;
(4) and performing de-bonding and air pressure sintering on the obtained silicon nitride biscuit to obtain the silicon nitride ceramic substrate.
2. The method according to claim 1, wherein the sintering aid is selected from MgO and Y 2 O 3 Or at least one of rare earth oxides; wherein the mass ratio of the raw material powder to the sintering aid is (75-97): (25-3), wherein the sum of the mass percentages of the two is 100 wt%; the rare earth oxide in the sintering aid accounts for 5-20 wt% of the total mass of the raw material powder and the sintering aid.
3. The production method according to claim 1, wherein the solvent is ethyl acetate, methyl ethyl ketone, or a mixed solvent of ethyl acetate and methyl ethyl ketone; when the solvent is a mixed solvent of ethyl acetate and butanone, the mass content of the butanone is 70-90 wt%, the mass content of the ethyl acetate is 10-30 wt%, and the sum of the mass percentages of the ethyl acetate and the ethyl acetate is 100 wt%; the mass of the solvent is 30-60 wt% of the total mass of the raw material powder and the sintering aid; when the raw material powder is silicon nitride powder, the mass of the solvent is preferably 40-50 wt%; when the raw material powder is silicon powder, the mass of the solvent is preferably 35-45 wt%.
4. The method according to any one of claims 1 to 3, wherein the silicon nitride powder has a particle size of 0.1 to 10 μm, the silicon powder has a particle size of 0.1 to 10 μm, and the sintering aid has a particle size of 0.1 to 10 μm.
5. The preparation method according to any one of claims 1 to 4, wherein the dispersant is at least one of castor oil, triolein and phosphate, and the addition amount is 0.5-10 wt% of the total mass of the raw material powder and the sintering aid;
the plasticizer is a mixture of butyl benzyl phthalate and polyethylene glycol-400, the total content of the plasticizer is 0.1-5 times of the binder content and is 1-5 wt% of the total mass of the raw material powder and the sintering aid, and the mass ratio of the butyl benzyl phthalate to the polyethylene glycol-400 is 0.1-5;
when the raw material powder is silicon nitride powder, the addition amount of the binder is 12-17 wt% of the total mass of the raw material powder and the sintering aid, and is preferably 13.5 wt%;
when the raw material powder is silicon powder, the addition amount of the binder is 12-15 wt%, preferably 13wt% of the total mass of the raw material powder and the sintering aid.
6. The preparation method according to any one of claims 1 to 5, wherein the rotation speed of the ball milling mixing is 10 to 500 rpm, and the total ball milling time is 48 to 144 hours;
the vacuum degree of the vacuum defoaming is less than or equal to 220mbar, the stirring speed is 10-50 r/min, and the defoaming time is 10-50 minutes;
the thickness of the green ceramic chip is 5-40 mm.
7. The preparation method according to any one of claims 1 to 6, wherein the atmosphere for de-bonding is vacuum, the temperature is 400 to 600 ℃, and the holding time is 1 to 24 hours; preferably, the temperature rise rate of the de-bonding is 1-10 ℃/min.
8. The production method according to any one of claims 1 to 7, wherein when the raw material powder contains silicon powder, after the debinding and before the air pressure sintering, the debinded silicon nitride biscuit is nitrided at 1200 to 1500 ℃ for 2 to 48 hours in a nitrogen atmosphere; preferably, the temperature rise rate of the nitriding treatment is 1-10 ℃/min.
9. The production method according to any one of claims 1 to 8, wherein the parameters of the gas pressure sintering include; the sintering atmosphere is nitrogen, the temperature is 1700-1900 ℃, the heat preservation time is 1-24 hours, and the air pressure is 0.1-10 MPa; preferably, the temperature rise rate and the temperature drop rate of the air pressure sintering are respectively 1-5 ℃/min.
10. A silicon nitride ceramic substrate prepared according to the preparation method described in any one of claims 1 to 9.
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| CN116462515A (en) * | 2023-03-13 | 2023-07-21 | 乐山职业技术学院 | Silicon nitride ceramic substrate and preparation method thereof |
| CN116639985A (en) * | 2023-06-07 | 2023-08-25 | 湖南湘瓷科艺有限公司 | High-thermal-conductivity silicon nitride ceramic substrate and application thereof |
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