CN113149661A - Preparation method of high-density boron nitride self-lubricating composite ceramic - Google Patents
Preparation method of high-density boron nitride self-lubricating composite ceramic Download PDFInfo
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- 239000002131 composite material Substances 0.000 title claims abstract description 62
- 239000000919 ceramic Substances 0.000 title claims abstract description 59
- 229910052582 BN Inorganic materials 0.000 title claims abstract description 48
- PZNSFCLAULLKQX-UHFFFAOYSA-N Boron nitride Chemical compound N#B PZNSFCLAULLKQX-UHFFFAOYSA-N 0.000 title claims abstract description 48
- 238000002360 preparation method Methods 0.000 title claims abstract description 10
- 239000000843 powder Substances 0.000 claims abstract description 33
- 238000005245 sintering Methods 0.000 claims abstract description 25
- 125000002887 hydroxy group Chemical group [H]O* 0.000 claims abstract description 22
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims abstract description 20
- 229910052782 aluminium Inorganic materials 0.000 claims abstract description 16
- 238000002156 mixing Methods 0.000 claims abstract description 16
- 239000002002 slurry Substances 0.000 claims abstract description 14
- 238000000498 ball milling Methods 0.000 claims abstract description 11
- 238000001035 drying Methods 0.000 claims abstract description 9
- 229910000831 Steel Inorganic materials 0.000 claims abstract description 8
- 239000010959 steel Substances 0.000 claims abstract description 8
- 238000003825 pressing Methods 0.000 claims abstract description 7
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 6
- 238000000280 densification Methods 0.000 claims abstract description 6
- 229910002804 graphite Inorganic materials 0.000 claims abstract description 6
- 239000010439 graphite Substances 0.000 claims abstract description 6
- 238000000034 method Methods 0.000 claims description 31
- 238000010438 heat treatment Methods 0.000 claims description 12
- 238000003756 stirring Methods 0.000 claims description 8
- 238000006243 chemical reaction Methods 0.000 claims description 7
- 238000001816 cooling Methods 0.000 claims description 7
- AZDRQVAHHNSJOQ-UHFFFAOYSA-N alumane Chemical class [AlH3] AZDRQVAHHNSJOQ-UHFFFAOYSA-N 0.000 claims description 6
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 6
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 5
- 239000012153 distilled water Substances 0.000 claims description 5
- 230000003301 hydrolyzing effect Effects 0.000 claims description 5
- 238000006116 polymerization reaction Methods 0.000 claims description 5
- 238000004321 preservation Methods 0.000 claims description 5
- 230000032683 aging Effects 0.000 claims description 4
- 238000001914 filtration Methods 0.000 claims description 4
- 239000000853 adhesive Substances 0.000 claims description 3
- 230000001070 adhesive effect Effects 0.000 claims description 3
- 239000004094 surface-active agent Substances 0.000 claims description 3
- JGDITNMASUZKPW-UHFFFAOYSA-K aluminium trichloride hexahydrate Chemical group O.O.O.O.O.O.Cl[Al](Cl)Cl JGDITNMASUZKPW-UHFFFAOYSA-K 0.000 claims description 2
- 229940009861 aluminum chloride hexahydrate Drugs 0.000 claims description 2
- 238000003760 magnetic stirring Methods 0.000 claims description 2
- 230000001050 lubricating effect Effects 0.000 abstract description 7
- 238000007789 sealing Methods 0.000 abstract description 6
- 239000003566 sealing material Substances 0.000 abstract description 6
- 238000005461 lubrication Methods 0.000 abstract description 4
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 abstract description 3
- 229910052593 corundum Inorganic materials 0.000 abstract description 3
- 229910001845 yogo sapphire Inorganic materials 0.000 abstract description 3
- VSCWAEJMTAWNJL-UHFFFAOYSA-K aluminium trichloride Chemical compound Cl[Al](Cl)Cl VSCWAEJMTAWNJL-UHFFFAOYSA-K 0.000 description 6
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 4
- 239000000203 mixture Substances 0.000 description 4
- 229920000036 polyvinylpyrrolidone Polymers 0.000 description 4
- 239000001267 polyvinylpyrrolidone Substances 0.000 description 4
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 description 4
- 238000010992 reflux Methods 0.000 description 4
- 239000000377 silicon dioxide Substances 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 description 2
- 239000004372 Polyvinyl alcohol Substances 0.000 description 2
- 229910052681 coesite Inorganic materials 0.000 description 2
- 229910052906 cristobalite Inorganic materials 0.000 description 2
- 238000001514 detection method Methods 0.000 description 2
- GVGUFUZHNYFZLC-UHFFFAOYSA-N dodecyl benzenesulfonate;sodium Chemical compound [Na].CCCCCCCCCCCCOS(=O)(=O)C1=CC=CC=C1 GVGUFUZHNYFZLC-UHFFFAOYSA-N 0.000 description 2
- 239000000314 lubricant Substances 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 229920002451 polyvinyl alcohol Polymers 0.000 description 2
- 239000011148 porous material Substances 0.000 description 2
- 238000001272 pressureless sintering Methods 0.000 description 2
- 229940080264 sodium dodecylbenzenesulfonate Drugs 0.000 description 2
- 238000002490 spark plasma sintering Methods 0.000 description 2
- 238000001228 spectrum Methods 0.000 description 2
- 229910052682 stishovite Inorganic materials 0.000 description 2
- 229910052905 tridymite Inorganic materials 0.000 description 2
- QYEXBYZXHDUPRC-UHFFFAOYSA-N B#[Ti]#B Chemical compound B#[Ti]#B QYEXBYZXHDUPRC-UHFFFAOYSA-N 0.000 description 1
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 description 1
- 229910052581 Si3N4 Inorganic materials 0.000 description 1
- 229910033181 TiB2 Inorganic materials 0.000 description 1
- 238000005411 Van der Waals force Methods 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 238000005054 agglomeration Methods 0.000 description 1
- 230000002776 aggregation Effects 0.000 description 1
- 239000012752 auxiliary agent Substances 0.000 description 1
- 238000005452 bending Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000002457 bidirectional effect Effects 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 238000009694 cold isostatic pressing Methods 0.000 description 1
- 238000009833 condensation Methods 0.000 description 1
- 230000005494 condensation Effects 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 238000007580 dry-mixing Methods 0.000 description 1
- 230000009977 dual effect Effects 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 238000001704 evaporation Methods 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000011268 mixed slurry Substances 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000012299 nitrogen atmosphere Substances 0.000 description 1
- 239000006259 organic additive Substances 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 229950008882 polysorbate Drugs 0.000 description 1
- 229920000136 polysorbate Polymers 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 238000000197 pyrolysis Methods 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 230000002194 synthesizing effect Effects 0.000 description 1
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N titanium dioxide Inorganic materials O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 1
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Abstract
The invention provides a preparation method of high-density boron nitride self-lubricating composite ceramic, which comprises the steps of mixing hBN powder with hydroxyl polymeric aluminum sol to form slurry with fluidity, performing ball milling and wet mixing on the slurry uniformly, and drying to obtain composite powder; then placing the composite powder in a steel mould and dry-pressing to form a boron nitride self-lubricating composite ceramic blank; and then placing the ceramic powder in a graphite mold, and performing pressure sintering densification by adopting discharge plasma in a vacuum environment to obtain the high-density boron nitride self-lubricating composite ceramic. The invention takes hydroxyl polymeric aluminum sol as a sintering aid to prepare hBN-Al2O3The density of the boron nitride self-lubricating composite ceramic of the system can reach 97 percent, and the boron nitride self-lubricating composite ceramic has excellent mechanical property and self-lubricating propertyThe lubricating performance can meet the requirements of mechanical equipment on high-speed operation and rotation of sealing components for lubrication and sealing materials.
Description
Technical Field
The invention relates to boron nitride composite ceramic, in particular to a preparation method of high-density boron nitride self-lubricating composite ceramic, which is used for meeting the requirements of mechanical equipment high-speed operation dynamic sealing components on lubricating and sealing materials.
Technical Field
Hexagonal boron nitride (hBN) is a stack of lamellar structures, and the layers are bonded with weak van der waals forces, and has excellent self-lubricating properties due to slippage under shear forces. Compared with other layered structure lubricants, the hBN has excellent high temperature resistance, the service temperature of the hBN in the air environment can reach more than 1000 ℃, and the hBN is a rare high-temperature solid lubricant and can meet the requirements of lubrication and dynamic sealing of moving parts of mechanical equipment in harsh environments.
As a self-lubricating sliding sealing material, not only is an excellent lubricating function required, but also internal pores of the material are reduced as much as possible, and sufficient strength is maintained so as to meet the requirements of high-speed operation of mechanical equipment on lubrication, sealing and service reliability. However, the B-N strong covalent bond bonding property, anisotropic plate structure and low self-diffusion coefficient of hBN make hBN ceramic composite materials difficult to densify, resulting in lower strength and carrying capacity, limiting their wide application.
Chinese patent CN 104193341A discloses a method for preparing high-purity hexagonal boron nitride ceramic by pressureless sintering, comprising the steps of firstly carrying out bidirectional pressurization and cold isostatic pressing on hBN powder, then presintering in air at 480-680 ℃, and finally carrying out pressureless sintering in nitrogen atmosphere at 2000-2200 ℃ for forming, wherein the density of the obtained boron nitride block is only about 58%, and the method has the disadvantages of too high sintering temperature, too large energy consumption and high production cost. At present, the compactness and mechanical property of sintering are improved by increasing sintering temperature and pressure, introducing various sintering aids or enhancing the same. The compactness of the hBN-based composite ceramic is related to not only the formula of the sintering aid, but also the introduction mode of an aid system. Chinese patent CN 1310149A discloses a method for synthesizing nitrogen by chemical reactionThe boron nitride-based composite ceramic is prepared with boron nitride powder, boron powder, titanium diboride powder and silica powder as material and through self-propagating reaction sintering process to synthesize BN-SiO2And BN-TiO2The density of the system composite ceramic is about 88%. The sintering aid of the boron nitride self-lubricating composite ceramic is of great importance, and unreasonable introduction can not only obtain a composite material with high density and ideal mechanical property, but also influence the exertion of the lubricating property.
Disclosure of Invention
In order to overcome the problem that the hBN self-lubricating composite ceramic is difficult to sinter and densify, the invention aims to provide a preparation method of the boron nitride self-lubricating composite ceramic, and the boron nitride self-lubricating composite ceramic with high compactness, excellent mechanical property and self-lubricating property is obtained so as to meet the requirements of mechanical equipment high-speed operation dynamic sealing components on lubricating and sealing materials.
Preparation of self-lubricating boron nitride composite ceramic
1. Preparation of sintering aid hydroxyl polymeric aluminum sol
Adding inorganic aluminum salt into distilled water, adding aluminum powder, and then forming sol containing hydroxyl polymeric aluminum through hydrolytic polymerization reaction. Wherein the inorganic aluminum salt is aluminum chloride hexahydrate; the mass ratio of the inorganic aluminum salt to the aluminum powder is 2: 1-3: 1. The concentration of Al in the hydroxyl polymeric aluminum sol is 2.0-3.5 mol/L.
And the hydrolytic polymerization reaction is carried out for 5-8 h by condensation and reflux under magnetic stirring at 80-100 ℃, and the homogeneous and transparent sol is obtained after the reaction is finished and the reaction is cooled to room temperature and filtered. The viscosity of the sol (viscosity is in the range of 30 to 60 mPas) can be adjusted by heating and evaporating.
In order to improve the cohesiveness of the hydroxyl polymeric aluminum sol, an adhesive which accounts for 0.5-1 wt% of the total mass of the sol can be added after the hydrolytic polymerization reaction, and the mixture is continuously stirred for 4-5 hours at the temperature of 50-70 ℃. The adhesive can adopt polyvinylpyrrolidone (PVP) or polyvinyl alcohol (PVA). Or heating and aging for 4-5 h at 50-70 ℃.
2. Preparation of self-lubricating boron nitride composite ceramic
(1) Mixing the hBN powder with the hydroxyl polymeric aluminum sol to form slurry with fluidity, performing ball milling and wet mixing to obtain uniformly mixed slurry, and drying the slurry to obtain the composite powder.
Wherein the molar ratio of the hBN to Al in the hydroxyl polymeric aluminum sol is 2: 1-5: 1. The size of the used hBN is 0.5-10 mu m, and the undersize or oversize is not beneficial to sintering densification and performance of lubricating performance.
When mixing, surfactants such as sodium dodecylbenzene sulfonate, polysorbate, etc. can be added to accelerate the mixing process. The addition amount of the surfactant is 0.05-0.2% of the mass of the hBN. Nanometer SiO with the mass of 5-30% of the hBN can also be added2Promotes the compactness of sintering. And an appropriate amount of absolute ethyl alcohol can be added to adjust the fluidity of the slurry and simultaneously contribute to accelerating the drying.
The ball milling time is 10-20 h, and the speed is 100-300 r/min. The drying temperature of the slurry is 50-80 ℃.
(2) And (2) placing the composite powder obtained in the step (1) in a steel die and performing dry pressing to form a boron nitride self-lubricating composite ceramic blank. Wherein the dry pressure intensity is 100-200 MPa, and the pressure maintaining time is 5-10 min.
(3) And (3) placing the boron nitride self-lubricating composite ceramic blank obtained in the step (2) in a graphite mold, and performing pressure sintering densification in a vacuum environment by adopting a spark plasma sintering technology (SPS).
The temperature rise rate in the sintering process is 100-150 ℃/min, the sintering temperature is 1500-1700 ℃, the pressure is 10-50 MPa, the heat preservation time is 5-10 min, and the vacuum degree is less than 100 Pa.
Structure and performance of boron nitride self-lubricating composite ceramic
FIG. 1 is a photograph of hydroxyl polyaluminum sol. It can be seen that the hydroxyl polyaluminium sol is homogeneous and transparent, and has uniform dispersion and certain viscosity.
FIG. 2 is an XRD spectrum of the boron nitride self-lubricating composite ceramic. XRD analysis shows that the self-lubricating composite boron nitride ceramic has hBN and Al as main components2O3And (4) forming.
FIG. 3 is a sectional view of the boron nitride self-lubricating composite ceramic. The sectional view shows that the hBN-Al prepared by the invention2O3The composite ceramic has compact and uniform structure, no obvious pores and Al2O3The grains are uniformly inserted between the hBN sheets.
Performance of self-lubricating boron nitride composite ceramic
1. Compactness degree
Detecting hBN-Al according to the standard GB/T25995-2O3Compactness of composite ceramic, and composite ceramic hBN-Al prepared by the invention2O3The density of the product can reach 97%.
2. Mechanical properties
The bending strength of the boron nitride self-lubricating composite ceramic is detected according to the national standards GB/T6569-2006/ISO 14704: 2000. The composite ceramic hBN-Al prepared by the invention2O3The strength of the steel is 70-100 MPa, and the steel has higher strength and bearing capacity.
3. Frictional properties
The tribology performance of a sample is tested by adopting a ball-disk type high-temperature frictional wear tester (HT-1000), the load is 5-10N, the frequency is 3-5 Hz, and the dual isΦ6 mm of Si3N4A ball. The self-lubricating composite ceramic hBN-Al prepared by the invention2O3The friction coefficient of (2) is 0.27-0.29, and the friction coefficient is stable in the friction process. The boron nitride self-lubricating composite ceramic prepared by the invention has good wear resistance.
In conclusion, the hydroxyl polyaluminium silicate sol is used as a sintering aid and is easy to enter between hBN sheets when being ball-milled and mixed with hBN, so that the problem of agglomeration or non-uniformity in the traditional dry mixing or wet mixing can be avoided, the hydroxyl polyaluminium silicate sol is fully and uniformly dispersed in the sol, the concentrated and dried powder has plasticity, the powder can be tightly bonded into a whole after dry pressing, and a compact blank body is more favorable for promoting the densification of the sintering process. In the sintering process, the hydroxy polymeric aluminum auxiliary agent forms Al mainly through the action of removing bound water2O3The ceramic and other added organic additives are also removed by pyrolysis, and finally homogeneous hBN-Al is obtained2O3The boron nitride self-lubricating composite ceramic of the system realizes the densification ceramic of hBN, and simultaneously endows the composite ceramic with excellent mechanical propertyThe lubricating and sealing material has self-lubricating performance, and can meet the requirements of mechanical equipment on lubrication and sealing materials for high-speed rotating sealing components.
Drawings
FIG. 1 is a photograph of hydroxyl polyaluminum sol.
FIG. 2 is an XRD spectrum of the boron nitride self-lubricating composite ceramic.
FIG. 3 is a sectional view of the boron nitride self-lubricating composite ceramic.
FIG. 4 is a friction coefficient curve of the boron nitride self-lubricating composite ceramic.
Detailed Description
The preparation and performance of the boron nitride self-lubricating composite ceramic of the present invention will be further explained by the following specific examples.
Example 1
9.657g of AlCl3·6H2Adding O into 85 mL of distilled water solution, magnetically stirring for 5 min, slowly adding 3.24g of Al powder, heating and stirring by an oil bath at 90 ℃, condensing and refluxing for 6 h, cooling to room temperature after the reaction is finished, and filtering to form homogeneous and transparent hydroxyl polymeric aluminum sol; adding a binding agent PVP (with the average molecular weight of 1300000 and the added mass fraction of 0.5 wt% of the total mass of the sol) into the sol, and heating and stirring the sol in an oil bath at 50 ℃ until the PVP is dissolved;
taking hBN powder with the particle size of about 5 mu m, adding a certain mass of sol, and enabling the molar ratio of hBN to Al in the sol to be 4.8: 1; then 10 g of absolute ethyl alcohol solution is added to form slurry with certain fluidity; ball milling and wet mixing for 20 h (ball milling speed 150 r/min), and drying the mixture into powder after uniform mixing;
loading the dried powder into a steel die, dry-pressing into a blank under 150 MPa, maintaining the pressure for 7 min, further transferring into a graphite die, and sintering by adopting discharge plasma under the conditions of 1600 ℃ and 35 MPa: the heating rate is 140 ℃/min, the heat preservation time is 8 min, and the boron nitride self-lubricating composite ceramic is obtained after cooling. The detection shows that the compactness is 85.2%, the strength is 70 MPa, the friction coefficient is about 0.27, the friction coefficient is stable in the friction process, and the friction coefficient curve is shown in figure 4 (a).
Example 2
9.657g of AlCl3·6H2Adding O into 85 mL of distilled water solution, magnetically stirring for 5 min, slowly adding 3.78g of Al powder, heating and stirring at 90 ℃ in an oil bath, condensing and refluxing for 5 h, cooling to room temperature after the reaction is finished, filtering, and heating and aging at 80 ℃ in the oil bath for 6 h to form homogeneous and transparent hydroxyl polymeric aluminum sol;
taking hBN powder with the grain diameter of about 1 mu m, adding sol with certain mass to ensure that the molar ratio of hBN to Al in the sol is 3:1, and then adding nano SiO2Powder (SiO)2The mass of the powder is 17 wt% of the total mass of the hBN), and 10 g of absolute ethyl alcohol solution is added to form slurry with certain fluidity; ball milling and wet mixing for 15 h (ball milling speed 200 r/min), and drying the mixture into powder after uniform mixing;
and (3) putting the dried powder into a steel die, dry-pressing the powder into a blank under 125 MPa, further transferring the blank into a graphite die, and sintering the blank by adopting discharge plasma under the conditions of 1700 ℃ and 35 MPa: the heating rate is 130 ℃/min, and the heat preservation time is 8 min; cooling to obtain hBN-Al2O3Self-lubricating composite ceramics. The detection shows that the density is 95.7%, the strength is 70 MPa, the sol friction coefficient is about 0.29, the friction coefficient is stable in the friction process, and the friction coefficient curve is shown in figure 4 (b).
Example 3
9.657g of AlCl3·6H2Adding O into 85 mL of distilled water solution, magnetically stirring for 5 min, slowly adding 4.32g of Al powder, heating and stirring at 90 ℃ in an oil bath, condensing and refluxing for 6 h, cooling to room temperature after the reaction is finished, filtering, and heating and aging at 80 ℃ in the oil bath for 6 h to form homogeneous and transparent hydroxyl polymeric aluminum sol;
taking hBN powder with the grain diameter of about 1 mu m, adding certain mass of sol, and enabling the molar ratio of hBN to Al in the sol to be 2: 1. In order to accelerate the mixing, sodium dodecyl benzene sulfonate (the addition amount is 0.1 wt% of the total mass of the hBN powder) is added, and 10 g of absolute ethyl alcohol solution is added to form slurry with certain fluidity; ball milling and wet mixing for 20 h (ball milling speed is 250 r/min), and drying the mixture into powder after uniform mixing;
and (3) putting the dried powder into a steel die, dry-pressing the powder into a blank under 175 MPa, further transferring the blank into a graphite die, and sintering the blank by adopting discharge plasma under the conditions of 1700 ℃ and 35 MPa: the heating rate is 120 ℃/min, the heat preservation time is 8 min, and the boron nitride self-lubricating composite ceramic is obtained after cooling. The density is 96.3%, the strength is 100 MPa, the friction coefficient is about 0.27, and the friction coefficient curve is shown in figure 4 (c).
Claims (10)
1. A preparation method of high-density boron nitride self-lubricating composite ceramic comprises the following steps:
(1) mixing the hBN powder with the hydroxyl polymeric aluminum sol to form slurry with fluidity, performing ball milling and wet mixing on the slurry uniformly, and drying to obtain composite powder;
(2) putting the composite powder obtained in the step (1) into a steel die and performing dry pressing to form a boron nitride self-lubricating composite ceramic blank; the dry pressure intensity is 100-200 MPa, and the pressure maintaining time is 5-10 min;
(3) placing the boron nitride self-lubricating composite ceramic blank obtained in the step (2) in a graphite mold, and performing pressure sintering densification by adopting discharge plasma in a vacuum environment to obtain high-density boron nitride self-lubricating composite ceramic; the temperature rise rate in the sintering process is 100-150 ℃/min, the sintering temperature is 1500-1700 ℃, the pressure is 10-50 MPa, the heat preservation time is 5-10 min, and the vacuum degree is less than 100 Pa.
2. The method for preparing the high-density boron nitride self-lubricating composite ceramic according to claim 1, wherein the method comprises the following steps: in the step (1), the hydroxyl polyaluminium sol is prepared by the following process: adding inorganic aluminum salt into distilled water, adding aluminum powder, performing hydrolytic polymerization reaction for 5-8 hours under magnetic stirring at 80-100 ℃, cooling to room temperature after the reaction is finished, and filtering to obtain homogeneous and transparent hydroxyl polymeric aluminum sol.
3. The method for preparing the high-density boron nitride self-lubricating composite ceramic according to claim 1, wherein the method comprises the following steps: in the step (1), the size of hBN is 0.5-10 μm; in the slurry, the molar ratio of the hBN to Al in the hydroxyl polymeric aluminum sol is 2: 1-5: 1.
4. The method for preparing the high-density boron nitride self-lubricating composite ceramic according to claim 1, wherein the method comprises the following steps: in the step (1), a surfactant which accounts for 0.05-0.2% of the mass of the hBN is added.
5. The method for preparing the high-density boron nitride self-lubricating composite ceramic according to claim 1, wherein the method comprises the following steps: in the step (1), nano SiO with the mass of 5-30% of hBN is added2Promotes the compactness of sintering.
6. The method for preparing the high-density boron nitride self-lubricating composite ceramic according to claim 1, wherein the method comprises the following steps: in the step (1), absolute ethyl alcohol is added to adjust the fluidity of the slurry.
7. The method for preparing the high-density boron nitride self-lubricating composite ceramic according to claim 1, wherein the method comprises the following steps: in the step (1), the ball milling time is 10-20 h, and the speed is 100-300 r/min.
8. The method for preparing the high-density boron nitride self-lubricating composite ceramic according to claim 1, wherein the method comprises the following steps: in the step (1), the drying temperature of the slurry is 50-80 ℃.
9. The method for preparing the high-density boron nitride self-lubricating composite ceramic according to claim 2, wherein the method comprises the following steps: the inorganic aluminum salt is aluminum chloride hexahydrate; the mass ratio of the inorganic aluminum salt to the aluminum powder is 2: 1-3: 1; the concentration of Al in the hydroxyl polymeric aluminum sol is 2.0-3.5 mol/L.
10. The method for preparing the high-density boron nitride self-lubricating composite ceramic according to claim 2, wherein the method comprises the following steps: adding an adhesive with the total mass of 0.5-1 wt% of the sol after the hydrolytic polymerization reaction, and continuously stirring for 4-5 h at 50-70 ℃; or heating and aging for 4-5 h at 50-70 ℃.
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