CN101817684B - Method for coating h-BN coating on surface of porous Si3N4 substrate - Google Patents

Method for coating h-BN coating on surface of porous Si3N4 substrate Download PDF

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CN101817684B
CN101817684B CN2010101324828A CN201010132482A CN101817684B CN 101817684 B CN101817684 B CN 101817684B CN 2010101324828 A CN2010101324828 A CN 2010101324828A CN 201010132482 A CN201010132482 A CN 201010132482A CN 101817684 B CN101817684 B CN 101817684B
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matrix
coating
ball
atmosphere
porous
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CN101817684A (en
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杨建锋
白宇
于方丽
梁森
乔冠军
张国军
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Xian Jiaotong University
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Xian Jiaotong University
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Abstract

The invention discloses a method for coating an h-BN coating on the surface of a porous Si3N4 substrate, which comprises the following steps of: 1, mixing Si3N4, Y2O3, Al2O3 and refinery coke in a mass ratio and grinding the mixture to prepare slurry; 2, drying and screening the slurry, pressing obtained powder into green compact and sintering the green compact in an N2 atmosphere to obtain the Si3N4 substrate; 3, washing and drying the Si3N4 substrate and coating H3BO3 onto the surface of the Si3N4 substrate; 4, heating the Si3N4 substrate coated with the H3BO3 and obtaining uniform B2O3 on the surface of the Si3N4 substrate; and 5, heating the Si3N4 substrate of which the surface has the B2O3 obtained in the step 4, and performing carbothermic reduction reaction to obtain the h-BN coating coated on the surface of the Si3N4 substrate. The method has the characteristics of low cost and simple operation; and a complex prepared structure integrates the advantages of two ceramic materials and can be widely applied to metal forming moulds.

Description

A kind of porous Si 3N 4Matrix surface covers the method that is coated with the h-BN coating
Technical field
The present invention relates to the method for porous matrix coating, particularly a kind of porous Si 3N 4Matrix surface covers the method that is coated with the h-BN coating.
Background technology
Porous Si 3N 4Pottery has good thermostability, corrosion resistance nature, antioxidant property and very high advantages such as physical strength as the structured material that high temperature uses down, aspect practical applications, demonstrates great potential and advantage.H-BN has the heat conductivility height, chemical property is stablized, almost all molten metals all is unreactiveness, resistance of oxidation is strong, thermostability is high and has performances such as very strong neutron receptivity and excellent electric insulating, so it has the high using value of potential in fields such as ceramic, fire-resistant, electrician, catalysis.The h-BN stupalith have very high thermal conductivity, excellent electric insulation performance, extremely low thermal expansivity and and the advantages such as not wellability of most metal, these character of himself have determined h-BN having rare advantage as advanced ceramic materials.But at present h-BN is relatively poor in ceramic mechanical property, also is not very extensive as the application of main components, does not have suitable method to come the h-BN of forms such as the particle of synthesis of nano yardstick, fiber and film in addition.In addition, because character such as the high-temperature stability of h-BN and low-down frictional coefficient make it in the high-temperature solid lubrication field, obtain using widely.As the h-BN of solid high temperature lubricant, it has higher heatproof characteristic and anti-portative power than some other lubricant, in corrosive atmosphere, also has advantages of higher stability, and nontoxic, look white, pollution-free etc. to environment and processed device.
Mostly that adopts at present the high-temperature chemical reaction preparation is the h-BN powder, as 1) inorganics and NH such as boron oxide compound, boron sodium salt 3Or N 2React; 2) borax, urea, two arteries and veins that contract, flesh, ammonia eyeball, Dyhard RU 100, sulphur arteries and veins or trimeric cyanamide etc. and NH 3Reaction; 3) boron simple substance and N 2Reaction etc.And high-quality h-BN coating adopts the vapour deposition process preparation more; These methods comprise chemical Vapor deposition process (CVD), Metalorganic Chemical Vapor Deposition (MOCVD), Low Pressure Chemical Vapor Deposition (LPCVD), ion assistance vapour deposition process (CVD of team), laser assistance vapour deposition process (LACVD) etc.; But the shortcoming of these methods is to cost an arm and a leg, complex process.
Summary of the invention
In order to overcome the defective of above-mentioned prior art, the object of the present invention is to provide a kind of porous Si 3N 4Matrix surface covers the method that is coated with the h-BN coating, utilizes the normal pressure-sintered porous silicon nitride ceramic sample of preparing, and guarantees the safety of matrix strength, utilizes H 3BO 3Decompose preparation B 2O 3Coating finally utilizes carbothermic reduction reaction with B 2O 3Coating changes the BN coating into, has guaranteed technologic stability, has low, the simple to operate characteristics of cost, and the composite structure of preparation combines the advantage of two kinds of stupaliths, can aspect metal molding die, be used widely.
In order to achieve the above object, technical scheme of the present invention is achieved in that
A kind of porous Si 3N 4Matrix surface covers the method that is coated with the h-BN coating, may further comprise the steps:
One, presses the Si of mass ratio with 30-50% 3N 4, 5%-7% Y 2O 3, 2%-6%A1 2O 3Mixing the ball grinder of packing into the refinery coke of 40-60%, is ball-milling medium with the absolute ethyl alcohol, with silicon nitride abrading-ball ball milling 24-48h, makes slip;
Two, with the slip that makes in 40-60 ℃ of loft drier dry 6-12 hour, cross 200 mesh sieves, obtain powder, the powder that obtains is pressed into the disk green compact, at N 21600 ℃ of-1800 ℃ of following sintering 2-3h in the atmosphere, N 2Pressure is 2-3 normal atmosphere, and obtaining void content is the Si of 25%-35% 3N 4Matrix;
Three, with the Si that sinters 3N 4Matrix is clean with surface cleaning with absolute ethyl alcohol, puts into drying baker 40-60 ℃ dry for standby then, again with the H of commercialization 3BO 3Evenly cover and be coated in Si 3N 4Matrix surface, required H 3BO 3Quality and Si 3N 4Surface of the base body is than being 0.2-0.6g/cm 2
Four, will cover and scribble H 3BO 3Si 3N 4Matrix is put into stove and is heated, and with the matrix 7-10 degree that tilts, Heating temperature is 500-700 ℃ during heating, and heating rate is 4-6 ℃/min, according to chemical equation 2H 3BO 3(S)=B 2O 3(s)+3H 2O (g) is at Si 3N 4Matrix surface obtains uniform B 2O 3
Five, surface in the step 4 had B 2O 3Si 3N 4Matrix is 4 atmospheric N at pressure 2Heat in the atmosphere, temperature is 1500 ℃-1700 ℃, utilizes carbothermic reduction reaction B 2O 3(s)+N 2(g)+and 3C (s) → 2BN (s)+3CO (g), form the h-BN coating, i.e. porous Si 3N 4Matrix surface covers and scribbles the h-BN coating.
The present invention utilizes porous Si 3N 4High temperature resistant, the pyrochemistry inertia that pottery and h-BN have reaches the not infiltrating characteristics with most metal, adopts simple carbon heat reducing to be reflected at porous Si 3N 4Matrix surface prepares the h-BN coating; It is being applied aspect accurate frock clamp of using in the glass-encapsulated of the smelting of non-ferrous metal and processing, glass melting and electron trade; For example this composite structure can be used as semi-conductor chip and outlet line welds, the ceramic welding mould of encapsulation usefulness; Be applicable to 600-950 ℃ of high-temperature soldering, encapsulation, and have high temperature medium-term and long-term use indeformable, the characteristics of sticking glass in the glass bulb encapsulation process; This composite structure also can be used as high technology ceramics mould and the frock clamp that the metallurgy of aluminium is used simultaneously, have aluminium liquid nonwetting, the characteristics of the long-term corrosion of anti-the aluminium alloy melt.The present invention has that cost is low, the measured characteristics of matter.
Description of drawings
Fig. 1 is embodiment 3B 2O 3Coating XRD figure spectrum.
Fig. 2 is that embodiment 3 carbothermic reduction temperature are the BN coating XRD figure spectrum under 1650 ℃.
Fig. 3 is that embodiment 3 carbothermic reduction temperature are the BN coating section SEM figure under 1650 ℃.
Fig. 4 is that embodiment 3 carbothermic reduction temperature are the BN coatingsurface SEM figure under 1650 ℃.
Embodiment
Embodiment one
Present embodiment may further comprise the steps:
One, presses mass ratio with 30% Si 3N 4, 5% Y 2O 3, 5%Al 2O 3Mixing the ball grinder of packing into 60% refinery coke, is ball-milling medium with the absolute ethyl alcohol, with silicon nitride abrading-ball ball milling 24h, makes slip;
Two, with the slip that makes in 40 ℃ of loft drier dry 12 hours, cross 200 mesh sieves, obtain powder, the powder that obtains is pressed into the disk green compact, at N 21600 ℃ of following sintering 2h in the atmosphere, N 2Pressure is 3 normal atmosphere, and the acquisition void content is 35% Si 3N 4Matrix;
Three, with the Si that sinters 3N 4Matrix is clean with surface cleaning with absolute ethyl alcohol, puts into 40 ℃ of dry for standby of drying baker then, again with the H of commercialization 3BO 3Evenly cover and be coated in Si 3N 4Matrix surface, required H 3BO 3Quality and Si 3N 4Surface of the base body is than being 0.2g/cm 2
Four, will cover and scribble H 3BO 3Si 3N 4Matrix is put into stove and is heated, and with matrix inclination 10 degree, Heating temperature is 700 ℃ during heating, and heating rate is 6 ℃/min, according to chemical equation 2H 3BO 3(S)=B 2O 3(s)+3H 2O (g) is at Si 3N 4Matrix surface obtains uniform B 2O 3
Five, surface in the step 4 had B 2O 3Si 3N 4Matrix is 4 atmospheric N at pressure 2Heat in the atmosphere, temperature is 1700 ℃, utilizes carbothermic reduction reaction B 2O 3(s)+N 2(g)+and 3C (s) → 2BN (s)+3CO (g), form the h-BN coating, i.e. porous Si 3N 4Matrix surface covers and scribbles the h-BN coating.
Embodiment two
Present embodiment may further comprise the steps:
One, presses mass ratio with 50% Si 3N 4, 4% Y 2O 3, 6%Al 2O 3Mixing the ball grinder of packing into 40% refinery coke, is ball-milling medium with the absolute ethyl alcohol, with silicon nitride abrading-ball ball milling 48h, makes slip;
Two, with the slip that makes in 60 ℃ of loft drier dry 6 hours, cross 200 mesh sieves, obtain powder, the powder that obtains is pressed into the disk green compact, at N 21800 ℃ of following sintering 2.8h in the atmosphere, N 2Pressure is 2 normal atmosphere, and the acquisition void content is 25% Si 3N 4Matrix;
Three, with the Si that sinters 3N 4Matrix is clean with surface cleaning with absolute ethyl alcohol, puts into 60 ℃ of dry for standby of drying baker then, again with the H of commercialization 3BO 3Evenly cover and be coated in Si 3N 4Matrix surface, required H 3BO 3Quality and Si 3N 4Surface of the base body is than being 0.3g/cm 2
Four, will cover and scribble H 3BO 3Si 3N 4Matrix is put into stove and is heated, and with matrix inclination 8 degree, Heating temperature is 500 ℃ during heating, and heating rate is 5 ℃/min, according to chemical equation 2H 3BO 3(S)=B 2O 3(s)+3H 2O (g) is at Si 3N 4Matrix surface obtains uniform B 2O 3
Five, surface in the step 4 had B 2O 3Si 3N 4Matrix is 4 atmospheric N at pressure 2Heat in the atmosphere, temperature is 1600 ℃, utilizes carbothermic reduction reaction B 2O 3(s)+N 2(g)+and 3C (s) → 2BN (s)+3CO (g), form the h-BN coating, i.e. porous Si 3N 4Matrix surface covers and scribbles the h-BN coating.
Embodiment three
Present embodiment may further comprise the steps:
One, presses mass ratio with 41% Si 3N 4, 5% Y 2O 3, 4%Al 2O 3Mixing the ball grinder of packing into 50% refinery coke, is ball-milling medium with the absolute ethyl alcohol, with silicon nitride abrading-ball ball milling 24h, makes slip;
Two, with the slip that makes in 50 ℃ of loft drier dry 9 hours, cross 200 mesh sieves, obtain powder, the powder that obtains is pressed into the disk green compact, at N 21650 ℃ of following sintering 3h in the atmosphere, N 2Pressure is 2 normal atmosphere, and the acquisition void content is 28% Si 3N 4Matrix;
Three, with the Si that sinters 3N 4Matrix is clean with surface cleaning with absolute ethyl alcohol, puts into 50 ℃ of dry for standby of drying baker then, again with the H of commercialization 3BO 3Evenly cover and be coated in Si 3N 4Matrix surface, required H 3BO 3Quality and Si 3N 4Surface of the base body is than being 0.6g/cm 2
Four, will cover and scribble H 3BO 3Si 3N 4Matrix is put into stove and is heated, and with matrix inclination 10 degree, Heating temperature is 600 ℃ during heating, and heating rate is 6 ℃/min, according to chemical equation 2H 3BO 3(S)=B 2O 3(s)+3H 2O (g) is at Si 3N 4Matrix surface obtains uniform B 2O 3
Five, surface in the step 4 had B 2O 3Si 3N 4Matrix is 4 atmospheric N at pressure 2Heat in the atmosphere, temperature is 1650 ℃, utilizes carbothermic reduction reaction B 2O 3(s)+N 2(g)+and 3C (s) → 2BN (s)+3CO (g), form the h-BN coating, i.e. porous Si 3N 4Matrix surface covers and scribbles the h-BN coating.
Fig. 1 is B in the present embodiment 2O 3Coating XRD figure spectrum, as can be seen from Figure 1, through preceding four steps of present embodiment, at Si 3N 4Matrix surface obtains B 2O 3Coating.
Fig. 2 is that the carbothermic reduction temperature is the coating XRD figure spectrum under 1650 ℃ in the present embodiment, as can be seen from Figure 2, through present embodiment at Si 3N 4Matrix surface obtains the h-BN coating, and Beta-Si is arranged 3N 4Appearance be because coating is thinner, X ray squeezes into that matrix causes.
Fig. 3 is that the carbothermic reduction temperature is the coating section SEM figure under 1650 ℃ in the present embodiment.As can be seen from Figure 3, the BN coat-thickness is approximately 1.6 μ m, the inner no significant defect of coating, and coating and matrix bond are better.
Fig. 4 is that the carbothermic reduction temperature is the BN coatingsurface SEM figure under 1650 ℃ in the present embodiment.As can beappreciated from fig. 4, BN coatingsurface opposed flattened, but have pit to occur, analyzing reason is because B 2O 3Vaporization at high temperature due to.
Embodiment four
Present embodiment may further comprise the steps:
One, presses mass ratio with 35% Si 3N 4, 7% Y 2O 3, 2%Al 2O 3Mixing the ball grinder of packing into 56% refinery coke, is ball-milling medium with the absolute ethyl alcohol, with silicon nitride abrading-ball ball milling 36h, makes slip;
Two, with the slip that makes in 45 ℃ of loft drier dry 10 hours, cross 200 mesh sieves, obtain powder, the powder that obtains is pressed into the disk green compact, at N 21700 ℃ of following sintering 2.5h in the atmosphere, N 2Pressure is 3 normal atmosphere, and the acquisition void content is 30% Si 3N 4Matrix;
Three, with the Si that sinters 3N 4Matrix is clean with surface cleaning with absolute ethyl alcohol, puts into 55 ℃ of dry for standby of drying baker then, again with the H of commercialization 3BO 3Evenly cover and be coated in Si 3N 4Matrix surface, required H 3BO 3Quality and Si 3N 4Surface of the base body is than being 0.4g/cm 2
Four, will cover and scribble H 3BO 3Si 3N 4Matrix is put into stove and is heated, and with matrix inclination 7 degree, Heating temperature is 650 ℃ during heating, and heating rate is 4 ℃/min, according to chemical equation 2H 3BO 3(S)=B 2O 3(s)+3H 2O (g) is at Si 3N 4Matrix surface obtains uniform B 2O 3
Five, surface in the step 4 had B 2O 3Si 3N 4Matrix is 4 atmospheric N at pressure 2Heat in the atmosphere, temperature is 1600 ℃, utilizes carbothermic reduction reaction B 2O 3(s)+N 2(g)+and 3C (s) → 2BN (s)+3CO (g), form the h-BN coating, i.e. porous Si 3N 4Matrix surface covers and scribbles the h-BN coating.
Embodiment five
Present embodiment may further comprise the steps:
One, presses mass ratio with 46% Si 3N 4, 6% Y 2O 3, 3%Al 2O 3Mixing the ball grinder of packing into 45% refinery coke, is ball-milling medium with the absolute ethyl alcohol, with silicon nitride abrading-ball ball milling 40h, makes slip;
Two, with the slip that makes in 55 ℃ of loft drier dry 8 hours, cross 200 mesh sieves, obtain powder, the powder that obtains is pressed into the disk green compact, at N 21750 ℃ of following sintering 2.2h in the atmosphere, N 2Pressure is 2.5 normal atmosphere, and the acquisition void content is 26% Si 3N 4Matrix;
Three, with the Si that sinters 3N 4Matrix is clean with surface cleaning with absolute ethyl alcohol, puts into 45 ℃ of dry for standby of drying baker then, again with the H of commercialization 3BO 3Evenly cover and be coated in Si 3N 4Matrix surface, required H 3BO 3Quality and Si 3N 4Surface of the base body is than being 0.5g/cm 2
Four, will cover and scribble H 3BO 3Si 3N 4Matrix is put into stove and is heated, and with matrix inclination 9 degree, Heating temperature is 550 ℃ during heating, and heating rate is 5.5 ℃/min, according to chemical equation 2H 3BO 3(S)=B 2O 3(s)+3H 2O (g) is at Si 3N 4Matrix surface obtains uniform B 2O 3
Five, surface in the step 4 had B 2O 3Si 3N 4Matrix is 4 atmospheric N at pressure 2Heat in the atmosphere, temperature is 1580 ℃, utilizes carbothermic reduction reaction B 2O 3(s)+N 2(g)+and 3C (s) → 2BN (s)+3CO (g), form the h-BN coating, i.e. porous Si 3N 4Matrix surface covers and scribbles the h-BN coating.

Claims (6)

1. porous Si 3N 4Matrix surface covers the method that is coated with the h-BN coating, it is characterized in that, may further comprise the steps:
One, presses the Si of mass ratio with 30-50% 3N 4, 5%-7% Y 2O 3, 2%-6%Al 2O 3Mixing the ball grinder of packing into the refinery coke of 40-60%, is ball-milling medium with the absolute ethyl alcohol, with silicon nitride abrading-ball ball milling 24-48h, makes slip;
Two, with the slip that makes in 40-60 ℃ of loft drier dry 6-12 hour, cross 200 mesh sieves, obtain powder, the powder that obtains is pressed into the disk green compact, at N 21600 ℃ of-1800 ℃ of following sintering 2-3h in the atmosphere, N 2Pressure is 2-3 normal atmosphere, and obtaining void content is the Si of 25%-35% 3N 4Matrix;
Three, with the Si that sinters 3N 4Matrix is clean with surface cleaning with absolute ethyl alcohol, puts into drying baker 40-60 ℃ dry for standby then, again with the H of commercialization 3BO 3Evenly cover and be coated in Si 3N 4Matrix surface, required H 3BO 3Quality and Si 3N 4Surface of the base body is than being 0.2-0.6g/cm 2
Four, will cover and scribble H 3BO 3Si 3N 4Matrix is put into stove and is heated, and with the matrix 7-10 degree that tilts, Heating temperature is 500-700 ℃ during heating, and heating rate is 4-6 ℃/min, according to chemical equation 2H 3BO 3(S)=B 2O 3(s)+3H 2O (g) is at Si 3N 4Matrix surface obtains uniform B 2O 3
Five, surface in the step 4 had B 2O 3Si 3N 4Matrix is 4 atmospheric N at pressure 2Heat in the atmosphere, temperature is 1500 ℃-1700 ℃, utilizes carbothermic reduction reaction B 2O 3(s)+N 2(g)+and 3C (s) → 2BN (s)+3CO (g), form the h-BN coating, i.e. porous Si 3N 4Matrix surface covers and scribbles the h-BN coating.
2. a kind of porous Si according to claim 1 3N 4Matrix surface covers the method that is coated with the h-BN coating, it is characterized in that, may further comprise the steps:
One, presses mass ratio with 30% Si 3N 4, 5% Y 2O 3, 5%Al 2O 3Mixing the ball grinder of packing into 60% refinery coke, is ball-milling medium with the absolute ethyl alcohol, with silicon nitride abrading-ball ball milling 24h, makes slip;
Two, with the slip that makes in 40 ℃ of loft drier dry 12 hours, cross 200 mesh sieves, obtain powder, the powder that obtains is pressed into the disk green compact, at N 21600 ℃ of following sintering 2h in the atmosphere, N 2Pressure is 3 normal atmosphere, and the acquisition void content is 35% Si 3N 4Matrix;
Three, with the Si that sinters 3N 4Matrix is clean with surface cleaning with absolute ethyl alcohol, puts into 40 ℃ of dry for standby of drying baker then, again with the H of commercialization 3BO 3Evenly cover and be coated in Si 3N 4Matrix surface, required H 3BO 3Quality and Si 3N 4Surface of the base body is than being 0.2g/cm 2
Four, will cover and scribble H 3BO 3Si 3N 4Matrix is put into stove and is heated, and with matrix inclination 10 degree, Heating temperature is 700 ℃ during heating, and heating rate is 6 ℃/min, according to chemical equation 2H 3BO 3(S)=B 2O 3(s)+3H 2O (g) is at Si 3N 4Matrix surface obtains uniform B 2O 3
Five, surface in the step 4 had B 2O 3Si 3N 4Matrix is 4 atmospheric N at pressure 2Heat in the atmosphere, temperature is 1700 ℃, utilizes carbothermic reduction reaction B 2O 3(s)+N 2(g)+and 3C (s) → 2BN (s)+3CO (g), form the h-BN coating, i.e. porous Si 3N 4Matrix surface covers and scribbles the h-BN coating.
3. a kind of porous Si according to claim 1 3N 4Matrix surface covers the method that is coated with the h-BN coating, it is characterized in that, may further comprise the steps:
One, presses mass ratio with 41% Si 3N 4, 5% Y 2O 3, 4%Al 2O 3Mixing the ball grinder of packing into 50% refinery coke, is ball-milling medium with the absolute ethyl alcohol, with silicon nitride abrading-ball ball milling 24h, makes slip;
Two, with the slip that makes in 50 ℃ of loft drier dry 9 hours, cross 200 mesh sieves, obtain powder, the powder that obtains is pressed into the disk green compact, at N 21650 ℃ of following sintering 3h in the atmosphere, N 2Pressure is 2 normal atmosphere, and the acquisition void content is 28% Si 3N 4Matrix;
Three, with the Si that sinters 3N 4Matrix is clean with surface cleaning with absolute ethyl alcohol, puts into 50 ℃ of dry for standby of drying baker then, again with the H of commercialization 3BO 3Evenly cover and be coated in Si 3N 4Matrix surface, required H 3BO 3Quality and Si 3N 4Surface of the base body is than being 0.6g/cm 2
Four, will cover and scribble H 3BO 3Si 3N 4Matrix is put into stove and is heated, and with matrix inclination 10 degree, Heating temperature is 600 ℃ during heating, and heating rate is 6 ℃/min, according to chemical equation 2H 3BO 3(S)=B 2O 3(s)+3H 2O (g) is at Si 3N 4Matrix surface obtains uniform B 2O 3
Five, surface in the step 4 had B 2O 3Si 3N 4Matrix is 4 atmospheric N at pressure 2Heat in the atmosphere, temperature is 1650 ℃, utilizes carbothermic reduction reaction B 2O 3(s)+N 2(g)+and 3C (s) → 2BN (s)+3CO (g), form the h-BN coating, i.e. porous Si 3N 4Matrix surface covers and scribbles the h-BN coating.
4. a kind of porous Si according to claim 1 3N 4Matrix surface covers the method that is coated with the h-BN coating, it is characterized in that, may further comprise the steps:
One, presses mass ratio with 35% Si 3N 4, 7% Y 2O 3, 2%Al 2O 3Mixing the ball grinder of packing into 56% refinery coke, is ball-milling medium with the absolute ethyl alcohol, with silicon nitride abrading-ball ball milling 36h, makes slip;
Two, with the slip that makes in 45 ℃ of loft drier dry 10 hours, cross 200 mesh sieves, obtain powder, the powder that obtains is pressed into the disk green compact, at N 21700 ℃ of following sintering 2.5h in the atmosphere, N 2Pressure is 3 normal atmosphere, and the acquisition void content is 30% Si 3N 4Matrix;
Three, with the Si that sinters 3N 4Matrix is clean with surface cleaning with absolute ethyl alcohol, puts into 55 ℃ of dry for standby of drying baker then, again with the H of commercialization 3BO 3Evenly cover and be coated in Si 3N 4Matrix surface, required H 3BO 3Quality and Si 3N 4Surface of the base body is than being 0.4g/cm 2
Four, will cover and scribble H 3BO 3Si 3N 4Matrix is put into stove and is heated, and with matrix inclination 7 degree, Heating temperature is 650 ℃ during heating, and heating rate is 4 ℃/min, according to chemical equation 2H 3BO 3(S)=B 2O 3(s)+3H 2O (g) is at Si 3N 4Matrix surface obtains uniform B 2O 3
Five, surface in the step 4 had B 2O 3Si 3N 4Matrix is 4 atmospheric N at pressure 2Heat in the atmosphere, temperature is 1600 ℃, utilizes carbothermic reduction reaction B 2O 3(s)+N 2(g)+and 3C (s) → 2BN (s)+3CO (g), form the h-BN coating, i.e. porous Si 3N 4Matrix surface covers and scribbles the h-BN coating.
5. a kind of porous Si according to claim 1 3N 4Matrix surface covers the method that is coated with the h-BN coating, it is characterized in that, may further comprise the steps:
One, presses mass ratio with 46% Si 3N 4, 6% Y 2O 3, 3%Al 2O 3Mixing the ball grinder of packing into 45% refinery coke, is ball-milling medium with the absolute ethyl alcohol, with silicon nitride abrading-ball ball milling 40h, makes slip;
Two, with the slip that makes in 55 ℃ of loft drier dry 8 hours, cross 200 mesh sieves, obtain powder, the powder that obtains is pressed into the disk green compact, at N 21750 ℃ of following sintering 2.2h in the atmosphere, N 2Pressure is 2.5 normal atmosphere, and the acquisition void content is 26% Si 3N 4Matrix;
Three, with the Si that sinters 3N 4Matrix is clean with surface cleaning with absolute ethyl alcohol, puts into 45 ℃ of dry for standby of drying baker then, again with the H of commercialization 3BO 3Evenly cover and be coated in Si 3N 4Matrix surface, required H 3BO 3Quality and Si 3N 4Surface of the base body is than being 0.5g/cm 2
Four, will cover and scribble H 3BO 3Si 3N 4Matrix is put into stove and is heated, and with matrix inclination 9 degree, Heating temperature is 550 ℃ during heating, and heating rate is 5.5 ℃/min, according to chemical equation 2H 3BO 3(S)=B 2O 3(s)+3H 2O (g) is at Si 3N 4Matrix surface obtains uniform B 2O 3
Five, surface in the step 4 had B 2O 3Si 3N 4Matrix is 4 atmospheric N at pressure 2Heat in the atmosphere, temperature is 1580 ℃, utilizes carbothermic reduction reaction B 2O 3(s)+N 2(g)+and 3C (s) → 2BN (s)+3CO (g), form the h-BN coating, i.e. porous Si 3N 4Matrix surface covers and scribbles the h-BN coating.
6. porous Si 3N 4Matrix surface covers the method that is coated with the h-BN coating, it is characterized in that, may further comprise the steps:
One, presses mass ratio with 50% Si 3N 4, 4% Y 2O 3, 6%Al 2O 3Mixing the ball grinder of packing into 40% refinery coke, is ball-milling medium with the absolute ethyl alcohol, with silicon nitride abrading-ball ball milling 48h, makes slip;
Two, with the slip that makes in 60 ℃ of loft drier dry 6 hours, cross 200 mesh sieves, obtain powder, the powder that obtains is pressed into the disk green compact, at N 21800 ℃ of following sintering 2.8h in the atmosphere, N 2Pressure is 2 normal atmosphere, and the acquisition void content is 25% Si 3N 4Matrix;
Three, with the Si that sinters 3N 4Matrix is clean with surface cleaning with absolute ethyl alcohol, puts into 60 ℃ of dry for standby of drying baker then, again with the H of commercialization 3BO 3Evenly cover and be coated in Si 3N 4Matrix surface, required H 3BO 3Quality and Si 3N 4Surface of the base body is than being 0.3g/cm 2
Four, will cover and scribble H 3BO 3Si 3N 4Matrix is put into stove and is heated, and with matrix inclination 8 degree, Heating temperature is 500 ℃ during heating, and heating rate is 5 ℃/min, according to chemical equation 2H 3BO 3(S)=B 2O 3(s)+3H 2O (g) is at Si 3N 4Matrix surface obtains uniform B 2O 3
Five, surface in the step 4 had B 2O 3Si 3N 4Matrix is 4 atmospheric N at pressure 2Heat in the atmosphere, temperature is 1600 ℃, utilizes carbothermic reduction reaction B 2O 3(s)+N 2(g)+and 3C (s) → 2BN (s)+3CO (g), form the h-BN coating, i.e. porous Si 3N 4Matrix surface covers and scribbles the h-BN coating.
CN2010101324828A 2010-03-25 2010-03-25 Method for coating h-BN coating on surface of porous Si3N4 substrate Expired - Fee Related CN101817684B (en)

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