CN111170743B - Silicon carbide infrared radiation ceramic material and preparation method thereof - Google Patents

Silicon carbide infrared radiation ceramic material and preparation method thereof Download PDF

Info

Publication number
CN111170743B
CN111170743B CN202010061183.3A CN202010061183A CN111170743B CN 111170743 B CN111170743 B CN 111170743B CN 202010061183 A CN202010061183 A CN 202010061183A CN 111170743 B CN111170743 B CN 111170743B
Authority
CN
China
Prior art keywords
powder
silicon carbide
ceramic material
infrared radiation
sio
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Active
Application number
CN202010061183.3A
Other languages
Chinese (zh)
Other versions
CN111170743A (en
Inventor
陈健
祝明
黄政仁
朱云洲
姚秀敏
陈忠明
刘学建
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Shanghai Institute of Ceramics of CAS
Original Assignee
Shanghai Institute of Ceramics of CAS
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Shanghai Institute of Ceramics of CAS filed Critical Shanghai Institute of Ceramics of CAS
Priority to CN202010061183.3A priority Critical patent/CN111170743B/en
Publication of CN111170743A publication Critical patent/CN111170743A/en
Application granted granted Critical
Publication of CN111170743B publication Critical patent/CN111170743B/en
Active legal-status Critical Current
Anticipated expiration legal-status Critical

Links

Images

Classifications

    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/515Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics
    • C04B35/56Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides
    • C04B35/565Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides based on silicon carbide
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/622Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30Constituents and secondary phases not being of a fibrous nature
    • C04B2235/38Non-oxide ceramic constituents or additives
    • C04B2235/3852Nitrides, e.g. oxynitrides, carbonitrides, oxycarbonitrides, lithium nitride, magnesium nitride
    • C04B2235/3865Aluminium nitrides
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/60Aspects relating to the preparation, properties or mechanical treatment of green bodies or pre-forms
    • C04B2235/602Making the green bodies or pre-forms by moulding
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/65Aspects relating to heat treatments of ceramic bodies such as green ceramics or pre-sintered ceramics, e.g. burning, sintering or melting processes
    • C04B2235/656Aspects relating to heat treatments of ceramic bodies such as green ceramics or pre-sintered ceramics, e.g. burning, sintering or melting processes characterised by specific heating conditions during heat treatment
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/65Aspects relating to heat treatments of ceramic bodies such as green ceramics or pre-sintered ceramics, e.g. burning, sintering or melting processes
    • C04B2235/656Aspects relating to heat treatments of ceramic bodies such as green ceramics or pre-sintered ceramics, e.g. burning, sintering or melting processes characterised by specific heating conditions during heat treatment
    • C04B2235/6567Treatment time
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/65Aspects relating to heat treatments of ceramic bodies such as green ceramics or pre-sintered ceramics, e.g. burning, sintering or melting processes
    • C04B2235/658Atmosphere during thermal treatment
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/65Aspects relating to heat treatments of ceramic bodies such as green ceramics or pre-sintered ceramics, e.g. burning, sintering or melting processes
    • C04B2235/658Atmosphere during thermal treatment
    • C04B2235/6581Total pressure below 1 atmosphere, e.g. vacuum
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/70Aspects relating to sintered or melt-casted ceramic products
    • C04B2235/74Physical characteristics
    • C04B2235/77Density
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/70Aspects relating to sintered or melt-casted ceramic products
    • C04B2235/96Properties of ceramic products, e.g. mechanical properties such as strength, toughness, wear resistance

Landscapes

  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Ceramic Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Structural Engineering (AREA)
  • Organic Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Ceramic Products (AREA)

Abstract

The invention relates to a silicon carbide infrared radiation ceramic material and a preparation method thereof, wherein the silicon carbide infrared radiation ceramic material comprises the following raw materials:β-SiC and MgO-Al2O3‑SiO2An auxiliary agent; preferably comprising: 76.5-95 wt% of beta-SiC, 0-8.5 wt% of AlN, 5-15 wt% of MgO-Al2O3‑SiO2And the sum of the contents of the components is 100 wt%.

Description

Silicon carbide infrared radiation ceramic material and preparation method thereof
Technical Field
The invention relates to a silicon carbide infrared radiation ceramic material and a preparation method thereof, in particular to a silicon carbide ceramic material with high infrared emissivity and a preparation method thereof, belonging to the field of infrared radiation ceramics.
Background
The infrared radiation ceramic material is an inorganic material with high emissivity or characteristic emissivity in an infrared band, and is an important functional material. The infrared radiation ceramic material has the characteristics of excellent infrared radiation performance, chemical stability, high-temperature stability and the like, and can be widely applied to the fields of infrared light sources, infrared heaters, thermophotovoltaic radiators, spacecraft thermal control coatings, satellite-borne microwave calibration sources, nuclear fusion calibration sources, LED heat dissipation substrates and the like.
For example: in a high-temperature furnace, most of heat transfer is caused by radiation, the high-emissivity coating is coated on the surface of a metal or refractory substrate, so that the heat radiation efficiency of the furnace can be effectively improved, the heat loss is obviously reduced, the tempering distribution in the furnace is more uniform, an infrared radiation coating material can play a role in protecting the substrate, the maintenance is reduced, and the service life of a furnace body is prolonged, the infrared radiation material developed by American CRC company can save energy by 10-30% when being applied to an industrial furnace, and meanwhile, the infrared radiation coating material can protect the substrate of a furnace lining to a certain extent, and the service life of the furnace lining can be prolonged by 1-4 times; in the field of hypersonic aircrafts, the hypersonic aerocraft has the outstanding characteristics that the heat transfer to the surface of the aerocraft is realized in the flying process, the heat energy can be reduced by increasing the radiation and conduction heat transfer of the surface, and the high emissivity material can play an effective role in the heat dissipation process; in addition, the infrared radiation coating with high emissivity can be used for the LED heat dissipation substrate to well solve the heat dissipation problem of a power LED, and the infrared radiation material can also be used as an antibacterial building material and has certain application in textiles.
In recent years, related research on infrared radiation materials is rapidly developed, wherein the emissivity of a wave band of 8-20 μm is over 0.9, while the radiation performance of the wave band of 1-8 μm is poor and is only about 0.5, and the emissivity is not high enough under a high temperature condition.
SiC has the advantages of high strength, high heat conductivity, high vacuum adaptability, high elastic modulus, low thermal expansion coefficient, excellent thermal shock resistance, corrosion resistance, oxidation resistance and the like, and is an important high-temperature structural material. SiC is a good infrared radiation material, has high infrared emissivity in all bands, and has high emissivity in the 2.5-8 mu m band. The SiC material has excellent performance and potential to be used as a better substitute in the application field of the existing infrared radiation material. However, the emissivity of the silicon carbide material in the middle band is low, and the lowest point is only about 0.2-0.3 at normal temperature, which is a problem that the SiC infrared radiation material needs to be solved urgently. For example, patent 1 (Chinese publication No. CN110078514A) discloses a silicon carbide ceramic with normal emissivity not less than 0.85 in the wavelength range of 1-22 μm. First, the emissivity is measured under high temperature, and the higher the temperature is, the larger the emissivity of the material is, and there is a large difference. Secondly, the tested wave band is 1-22 μm, and the emissivity of the silicon carbide after the wave band is 15 microns is very high and is close to 1, so that the total emissivity is greatly improved to a certain extent. In fact, the silicon carbide obtained in patent 1 is still low (e.g. only 0.69) at 2.5-16 μm.
Disclosure of Invention
Aiming at the problems, the invention aims to provide a silicon carbide ceramic infrared radiation material with high mid-band emissivity and a preparation method thereof.
In one aspect, the invention provides a silicon carbide infrared radiation ceramic material, which comprises the following raw materials: beta-SiC and MgO-Al2O3-SiO2An auxiliary agent; preferably comprising: 76.5-95 wt% of beta-SiC, 0-8.5 wt% of AlN, 5-15 wt% of MgO-Al2O3-SiO2And the sum of the contents of the components is 100 wt%.
Preferably, the MgO-Al2O3-SiO2The auxiliary agent comprises the following raw material components: 10 to 30wt% of MgO and 15 to 40wt% of Al2O3、20~60wt%SiO2The sum of the contents of all the components is 100 wt%.
Preferably, the silicon carbide infrared radiation ceramic material comprises the following raw materials: 80-90 wt% of beta-SiC, 0-6 wt% of AlN, and 5-15 wt% of MgO-Al2O3-SiO2And the sum of the contents of the components is 100 wt%.
Preferably, the silicon carbide infrared radiation ceramic material has an infrared emissivity of 0.75-0.84 at a normal temperature of 2.5-16 μm; the density of the silicon carbide infrared radiation ceramic material is 2.01-2.50 g/cm3The bending strength is 68-210 MPa.
On the other hand, the invention provides a preparation method of the silicon carbide infrared radiation ceramic material, which comprises the following steps:
(1) selecting beta-SiC powder and AlN powder as raw material powder, mixing, and carrying out solid solution reaction at 1700-2000 ℃ to obtain solid solution powder;
(2) mixing the obtained solid solution powder with MgO-Al2O3-SiO2Mixing the auxiliary agents to obtain mixed powder;
(3) and pressing and molding the obtained mixed powder, and then performing vacuum de-bonding and sintering to obtain the silicon carbide ceramic material with high infrared emissivity.
In the invention, firstly, the beta-SiC powder and the AlN powder are subjected to solid solution reaction at 1700-2000 ℃ so that the AlN powder is firstly dissolved in the beta-SiC powder in a solid solution way,to avoid the subsequent vacuum debonding and sintering process with MgO-Al2O3-SiO2The oxides of all the components in the auxiliary agent react. Further, the introduction of an AlN impurity element into an SiC crystal destroys the lattice periodicity, resulting in a decrease in the symmetry of lattice vibration, while the enhancement of non-simple harmonic vibration widens the vibration absorption band, thereby promoting the vibration absorption of the lattice. Meanwhile, the existence of the AlN impurity element causes the electronic energy states of the regions to be different from those of other regions, and is favorable for forming impurity energy levels in forbidden band gaps of electrons. The formation of the impurity energy level can provide convenient conditions for the transition of holes and electrons in a valence band, so that the concentration of free carriers in the crystal can be improved, the infrared absorption of the free carriers in the SiC crystal can be improved, namely, the infrared absorption performance of the crystal is improved, and the crystal is formed by the kirchhoff law:
Figure BDA0002374549970000021
it is known that a good absorber is necessarily a good radiator, and thus, the infrared emissivity of the material is improved. Then solid solution powder and MgO-Al are mixed2O3-SiO2Mixing the auxiliary agents, pressing and forming, and then carrying out vacuum de-bonding and sintering. MgO-Al of specific composition during sintering2O3-SiO2The system can further form cordierite dispersed in the SiC matrix, and the cordierite with high emissivity in a wave band of 8-14 mu m is further realized, namely a material compounding method is adopted, so that the silicon carbide infrared radiation ceramic material can be in different temperature ranges and different wavelength ranges, and the infrared radiation capability of the material is complemented and enhanced.
Preferably, the mass contents of the beta-SiC powder and the AlN powder are respectively 90-100 wt% and 0-10 wt%, and the sum of the mass percentages is 100wt%, which is calculated according to the raw material components of the silicon carbide infrared radiation ceramic material.
Preferably, the solid solution powder and MgO-Al are calculated according to the raw material components of the silicon carbide infrared radiation ceramic material2O3-SiO2Mass content of the auxiliary85-95 wt% and 5-15 wt% respectively, and the sum of the mass percentages is 100 wt%.
Preferably, according to MgO-Al2O3-SiO2Raw material components of the auxiliary agent are weighed MgO powder and Al2O3Powder and SiO2Mixing the powder to obtain the MgO-Al2O3-SiO2And (4) an auxiliary agent.
Preferably, the grain diameter of the beta-SiC powder is 0.5 to 1 mu m; the particle size of the AlN powder is 1-2 mu m; the particle size of the MgO powder is 1-3 μm; the Al is2O3The particle size of the powder is 100-200 nm; the SiO2The particle size of the powder is 1 to 3 μm.
Preferably, the atmosphere of the solid solution reaction is an inert atmosphere, preferably an argon atmosphere; the gas pressure of the solid solution reaction is 40-75 mbar; the time of the solid solution reaction is 2-4 hours.
Preferably, the raw material powder or the mixed powder further comprises a binder; the binder is selected from at least one of phenolic resin, polyvinyl alcohol PVA and polyvinyl butyral PVB; the addition amount of the binder is not more than 8wt% of the total mass of the raw material powder. The binder is added into the raw material powder, so that the binder and the raw material powder are uniformly mixed and simultaneously wrapped on the surfaces of the beta-SiC powder and the AlN powder, the binder is used as a carbon source to be cracked in the subsequent solid solution reaction process to generate nano-scale residual carbon, the carbon and a silicon dioxide layer on the surface of the silicon carbide powder are subjected to reduction reaction to generate silicon carbide and carbon monoxide gas, aluminum nitride is in contact with the surface of fresh silicon carbide powder and further promotes the solid solution reaction to enter a silicon carbide lattice, and the XRD result has no AlN characteristic peak as can be proved in figure 1.
Preferably, the compression molding mode is dry compression molding or/and cold isostatic pressing, and preferably, the dry compression molding is performed before the cold isostatic pressing.
Preferably, the pressure of the dry pressing is 5 to 20MPa, and the pressure of the cold isostatic pressing is 180 to 200 MPa.
Preferably, the temperature of the vacuum de-bonding is 700-1000 ℃, the time is 0.5-2 hours, and the vacuum degree is-5-10 Pa.
Preferably, the sintering atmosphere is an inert atmosphere, preferably an argon atmosphere; the pressure of the inert atmosphere is 40-75 mbar; the sintering temperature is 1400-1950 ℃; the sintering time is 1-3 hours.
Has the advantages that:
in the invention, the silicon carbide infrared radiation ceramic material has higher infrared emissivity, and is sintered at low temperature to obtain a product, thereby greatly reducing the cost investment. At the same time, doped MgO-Al2O3-SiO2The cordierite structure formed by the system enables the prepared silicon carbide material to have a lower thermal expansion coefficient and a higher thermal conductivity, and the prepared silicon carbide ceramic has certain strength and wide application prospect.
Drawings
FIG. 1 is an XRD spectrum of solid solution powders with different AlN contents obtained at 2000 ℃, wherein, no AlN peak is found in the XRD spectrum of the powders with different AlN contents, thus showing that AlN is solid dissolved in the silicon carbide crystal lattice;
FIG. 2 is a chart showing the IR emissivity of SiC IR-radiation ceramic material prepared from the solid solution powder of AlN at 1950 deg.C, in which MgO-Al is shown2O3-SiO2The emissivity of the silicon carbide ceramic prepared by the system with the sintering aid is greatly improved (the silicon carbide ceramic can be distinguished from the lowest point, and the lowest emissivity value of intrinsic silicon carbide ceramic is 0.2-0.3), and the emissivity of the silicon carbide ceramic is improved to a certain extent by introducing AlN;
FIG. 3 is a chart showing the infrared emissivity of a silicon carbide infrared radiation ceramic material prepared by solid solution powders with different AlN contents at 1480 ℃ at normal temperature, and comparing with FIG. 2, it can be seen that the emissivity difference still exists whether AlN is doped or not, and the difference is that all the emissivity is improved compared with that at 1950 ℃.
Detailed Description
The present invention is further illustrated by the following examples, which are to be understood as merely illustrative and not restrictive.
Book of JapaneseIn the beginning, the raw material components of the silicon carbide infrared radiation ceramic material comprise: 76.5 to 95wt% of beta-SiC, 0 to 8.5wt% of AlN, and 5 to 15wt% of MgO-Al2O3-SiO2And the sum of the contents of the components is 100 wt%. Wherein, MgO-Al2O3-SiO2The auxiliary agent is MgO and Al2O3And SiO2The mixed powder of (1). Preferably, MgO-Al2O3-SiO2The auxiliary agent comprises the following raw material components: 10 to 30wt% of MgO and 15 to 40wt% of Al2O3、20~60wt%SiO2The sum of the contents of all the components is 100 wt%.
In an alternative embodiment, the feedstock composition of the silicon carbide infrared radiating ceramic material preferably comprises: 80-90 wt% of SiC, 0-6 wt% of AlN, and 5-15 wt% of MgO-Al2O3-SiO2The sum of the contents of all the components is 100 percent.
In one embodiment of the present invention, the beta-SiC powder and the AlN powder are subjected to a solid solution reaction under normal pressure sintering conditions, and MgO-Al is used2O3-SiO2The system is used as a sintering aid and added into the powder prepared by the solid solution reaction for normal pressure sintering to obtain the silicon carbide infrared radiation ceramic material with excellent performance. The preparation method of the silicon carbide infrared radiation ceramic material provided by the invention is exemplarily described below.
Mixing 90-100 wt% of beta-SiC powder and 0-10 wt% of AlN powder according to different proportions, and simultaneously adding absolute ethyl alcohol as a solvent for ball milling to obtain mixed slurry 1 with the solid content of 40-50 wt%. And directly drying the mixed slurry 1 or performing spray granulation to obtain powder to be solid-dissolved (raw material powder). In the ball milling process, SiC balls with certain gradation are added as ball milling media, and the ball milling time can be 12 hours. The grain diameter of the beta-SiC powder can be 0.5-1 mu m. The AlN powder has a particle size of 1 to 2 μm.
In an alternative embodiment, in the mixed slurry 1, a binder is preferably added as a carbon source in an amount of 0 to 8wt% (preferably 0 to 6 wt%) based on the total mass of the raw material powder to promote the solid solution reaction. The binder may be at least one of phenolic resin, polyvinyl alcohol PVA, and polyvinyl butyral PVB. Wherein the binder may be added in the form of a solution, such as a phenolic resin solution.
And placing the powder to be solid-dissolved in a high-purity graphite crucible, and carrying out solid-solution reaction in a normal-pressure sintering furnace to obtain the solid-solution powder. Wherein the specific parameters of the solid solution reaction are as follows: the temperature of the solid solution reaction is controlled to be 1800-2000 ℃, the heat preservation time is 2-4 h, and the furnace pressure is controlled to be 40-75 mbar in an inert atmosphere (such as argon atmosphere). Preferably, the temperature rise rate in the solid solution reaction process is 2-8 ℃/min. If the AlN powder and the MgO-Al are directly added into the beta-silicon carbide at the same time2O3-SiO2And the AlN powder is wrapped by the oxide assistant and cannot reach the preliminarily designed solid solution in the silicon carbide crystal lattice.
10-30 wt% of MgO and 15-40 wt% of Al are taken2O3、20~60wt%SiO2Mixing the powder, adding absolute ethyl alcohol, and performing ball milling by using SiC balls for 6-12 hours to obtain mixed slurry 2. Placing the obtained mixed slurry 2 in an oven, drying for 12-24 hours at 70 ℃, and sieving the dried slurry with a sieve of 80-120 meshes to obtain MgO-Al2O3-SiO2And (4) an auxiliary agent. The particle size of the MgO powder may be 1 to 3 μm. Al (Al)2O3The particle size of the powder can be 100-200 nm. SiO 22The particle size of the powder can be 1-3 μm.
Selecting solid solution powder obtained by 85-95 wt% of solid solution reaction and 5-15 wt% of MgO-Al2O3-SiO2The system liquid phase auxiliary agent is taken as a raw material, a proper amount of absolute ethyl alcohol is added, and ball milling and mixing are carried out to obtain mixed slurry 2. And drying and sieving the obtained mixed slurry 2 to obtain mixed powder. For example, the mixed slurry 2 is put in an oven, dried at 70 ℃ for 12 hours, and the dried slurry is passed through a 100-mesh sieve to obtain a mixed powder. In the ball milling process, SiC balls with certain gradation are also used for ball milling, and the ball milling time can be 12 hours.
In an alternative embodiment, a binder is preferably added to the mixed slurry 2 in an amount of 0 to 8wt% (preferably 0 to 6 wt%) based on the total mass of the mixed powder. The binder may be at least one of phenolic resin, polyvinyl alcohol PVA, and polyvinyl butyral PVB. Wherein the binder may be added in the form of a solution, such as a phenolic resin solution.
And directly pressing and molding the mixed powder to obtain a blank. Wherein the compression molding mode can be dry compression molding or/and cold isostatic pressing. Wherein, the pressure of dry pressing molding can be 5-20 MPa. The pressure of the cold isostatic pressing can be 180-200 MPa. As an example of the press molding of a blank, dry press molding is performed at a pressure of 5 to 20MPa, and then cold isostatic pressing is performed at a pressure of 180 to 200MPa, wherein the medium of the cold isostatic pressing is oil or water.
And placing the blank into a high-purity graphite crucible, and performing vacuum debonding in a normal-pressure debonding furnace. The specific parameters of the vacuum debonding process are as follows: controlling the de-bonding temperature to be 700-1000 ℃, the heat preservation time to be 0.5-2 h, and controlling the furnace pressure to be-5-10 Pa.
Placing the blank after vacuum debonding in a high-purity graphite crucible, and adopting a powder embedding process to contain 10-20 wt% of MgO-Al2O3-SiO2And (3) wrapping the vacuum-debonded green body with SiC powder of the system liquid phase auxiliary agent, and further placing the green body in a normal-pressure sintering furnace for sintering to prepare the silicon carbide ceramic material with high infrared emissivity. Wherein, the sintering process parameters comprise: controlling the sintering temperature to 1400-1950 ℃, the heat preservation time to 1-3 h, and controlling the furnace pressure to 40-75 mbar in an inert atmosphere (such as argon atmosphere).
According to the invention, the obtained silicon carbide ceramic material has high infrared emissivity, and the normal-temperature normal infrared emissivity of the silicon carbide ceramic material can be 0.75-0.84 in a spectral range of 2.5-16 mu m by testing with an IR-2 dual-band emissivity tester. The density of the silicon carbide infrared radiation ceramic material measured by an Archimedes drainage method can be 2.01-2.50 g/cm3. The bending strength of the prepared silicon carbide infrared radiation ceramic material measured by a three-point bending method can be 68-210 MPa.
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, which is defined by the appended claimsThe invention is intended to cover by the appended claims some insubstantial modifications and adaptations of the invention. 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. In the following examples, MgO-Al is mentioned, unless otherwise specified2O3-SiO2The ball milling and mixing process of the auxiliary agent comprises the following steps: taking 20 wt% MgO and 25 wt% Al2O3、55wt%SiO2Mixing the powder, adding absolute ethyl alcohol, and performing ball milling by using SiC balls for 12 hours; placing the obtained mixed slurry in an oven, drying for 12 hours at 70 ℃, sieving the dried slurry with a 100-mesh sieve to obtain MgO-Al2O3-SiO2Liquid phase system assistant (MgO-Al for short)2O3-SiO2Auxiliaries), i.e., MgO, Al2O3And SiO2The mixed powder of (1).
Example 1
Taking 200g of 100wt% beta-SiC and 0wt% AlN, and 4g of phenolic resin, using SiC balls with a certain gradation as a ball milling medium, adding absolute ethyl alcohol as a solvent, carrying out ball milling for 12 hours, drying and sieving to obtain raw material powder;
putting the obtained raw material powder into a normal pressure sintering furnace, carrying out solid solution reaction under the argon atmosphere, controlling the temperature to be 2000 ℃, and keeping the temperature for 3 hours to obtain SiC powder;
90g of the SiC powder was taken, and 10g of the MgO-Al powder obtained above was added2O3-SiO2Adding an auxiliary agent, namely adding 2g of phenolic resin, using SiC balls with a certain gradation as a ball milling medium, adding absolute ethyl alcohol as a solvent, carrying out ball milling for 12 hours, drying and sieving, forming the obtained powder on a manual hydraulic press at the pressure of 8MPa, and then carrying out isostatic pressing at the pressure of 200MPa to obtain a blank;
and (3) performing vacuum de-bonding on the obtained blank (the temperature is 900 ℃, and the heat preservation time is 0.5 hour), placing the blank into a normal-pressure sintering furnace, sintering in the argon atmosphere, controlling the sintering temperature to 1950 ℃, preserving the heat for 2 hours, controlling the temperature to 1300 ℃ by a program, preserving the heat for 2 hours, and then cooling along with the furnace, and grinding the obtained silicon carbide ceramic wafer to obtain the silicon carbide infrared radiation ceramic material.
The silicon carbide infrared radiation ceramic material has a normal temperature normal infrared emissivity of 0.75 in a spectral range of 2.5-16 mu m by an IR-2 dual-waveband emissivity measuring instrument. The bending strength of the prepared silicon carbide infrared radiation ceramic material test strip (3mm multiplied by 4mm multiplied by 36mm) measured by a three-point bending method is 205 MPa. The density of the silicon carbide infrared radiation ceramic material measured by an Archimedes drainage method is 2.47g/cm3
Example 2
Taking 200g of 96 wt% of beta-SiC and 4 wt% of AlN, taking 4g of phenolic resin, using SiC balls with a certain gradation as a ball milling medium, adding absolute ethyl alcohol as a solvent, carrying out ball milling for 12 hours, drying and sieving to obtain raw material powder;
putting the obtained raw material powder into a normal pressure sintering furnace, carrying out solid solution reaction under the atmosphere of argon, controlling the temperature to be 2000 ℃, and keeping the temperature for 3 hours to obtain SiC-AlN solid solution powder;
90g of the SiC-AlN solid solution powder was taken, and 10g of the MgO-Al obtained above was added2O3-SiO2Adding an auxiliary agent, namely adding 2g of phenolic resin, using SiC balls with a certain gradation as a ball milling medium, adding absolute ethyl alcohol as a solvent, carrying out ball milling for 12 hours, drying and sieving, forming the obtained powder on a manual hydraulic press at the pressure of 8MPa, and then carrying out cold isostatic pressing at the pressure of 200MPa to obtain a blank;
and (3) performing vacuum de-bonding on the obtained blank (the temperature is 900 ℃, and the heat preservation time is 0.5 hour), placing the blank into a normal-pressure sintering furnace, sintering in the argon atmosphere, controlling the sintering temperature to 1950 ℃, preserving the heat for 2 hours, controlling the temperature to 1300 ℃ by a program, preserving the heat for 2 hours, and then cooling along with the furnace, and grinding the obtained silicon carbide ceramic wafer to obtain the silicon carbide infrared radiation ceramic material.
The silicon carbide infrared radiation ceramic material has a normal temperature normal infrared emissivity of 0.79 within a spectral range of 2.5-16 mu m through the test of an IR-2 dual-waveband emissivity measuring instrument. The silicon carbide infrared radiation ceramic material (size 3 mm. times.4 mm. times.36 mm) had a flexural strength of 157MPa as measured by a three-point bending method. Measured by Archimedes drainage methodThe density of the silicon carbide infrared radiation ceramic material is 2.33g/cm3
Example 3
Taking 200g of 100wt% beta-SiC and 0wt% AlN, and 4g of phenolic resin, using SiC balls with a certain gradation as a ball milling medium, adding absolute ethyl alcohol as a solvent, carrying out ball milling for 12 hours, drying and sieving to obtain raw material powder;
putting the obtained raw material powder into a normal pressure sintering furnace, carrying out solid solution reaction under the argon atmosphere, controlling the temperature to be 2000 ℃, and keeping the temperature for 3 hours to obtain SiC powder;
90g of the SiC powder was taken, and 10g of the MgO-Al powder obtained above was added2O3-SiO2Adding an auxiliary agent, namely adding 2g of phenolic resin, using SiC balls with a certain gradation as a ball milling medium, adding absolute ethyl alcohol as a solvent, carrying out ball milling for 12 hours, drying and sieving, forming the obtained powder on a manual hydraulic press at the pressure of 8MPa, and then carrying out cold isostatic pressing at the pressure of 200MPa to obtain a blank;
and (3) after vacuum de-bonding (the temperature is 900 ℃ and the heat preservation time is 0.5 hour), placing the obtained blank in a normal-pressure sintering furnace, sintering in the argon atmosphere, controlling the sintering temperature to 1480 ℃ and the heat preservation time to be 2 hours, controlling the temperature to 1300 ℃ by a program, preserving the heat for 2 hours, and then cooling along with the furnace, grinding the obtained silicon carbide ceramic wafer to obtain the silicon carbide infrared radiation ceramic material.
The silicon carbide infrared radiation ceramic material has a normal temperature normal infrared emissivity of 0.82 in a spectral range of 2.5-16 mu m through the test of an IR-2 dual-waveband emissivity measuring instrument. The silicon carbide infrared radiation ceramic material (3 mm. times.4 mm. times.36 mm in size) had a bending strength of 68MPa as measured by a three-point bending method. The density of the silicon carbide infrared radiation ceramic material measured by an Archimedes drainage method is 2.01g/cm3
Example 4
Taking 200g of 96 wt% of beta-SiC and 4 wt% of AlN, taking 4g of phenolic resin, using SiC balls with a certain gradation as a ball milling medium, adding absolute ethyl alcohol as a solvent, carrying out ball milling for 12 hours, drying and sieving to obtain raw material powder;
putting the obtained raw material powder into a normal pressure sintering furnace, carrying out solid solution reaction under the atmosphere of argon, controlling the temperature to be 2000 ℃, and keeping the temperature for 3 hours to obtain SiC-AlN solid solution powder;
90g of the SiC-AlN solid solution powder was taken, and 10g of the MgO-Al obtained above was added2O3-SiO2Adding an auxiliary agent, namely adding 2g of phenolic resin, using SiC balls with a certain gradation as a ball milling medium, adding absolute ethyl alcohol as a solvent, carrying out ball milling for 12 hours, drying and sieving, forming the obtained powder on a manual hydraulic press at the pressure of 8MPa, and then carrying out cold isostatic pressing at the pressure of 200MPa to obtain a blank;
and (3) after vacuum de-bonding (the temperature is 900 ℃ and the heat preservation time is 0.5 hour), placing the obtained blank in a normal-pressure sintering furnace, sintering in the argon atmosphere, controlling the sintering temperature to 1480 ℃ and the heat preservation time to be 2 hours, controlling the temperature to 1300 ℃ by a program, preserving the heat for 2 hours, and then cooling along with the furnace, grinding the obtained silicon carbide ceramic wafer to obtain the silicon carbide infrared radiation ceramic material.
The silicon carbide infrared radiation ceramic material has a normal temperature normal infrared emissivity of 0.84 in a spectral range of 2.5-16 mu m by an IR-2 dual-waveband emissivity measuring instrument. The silicon carbide infrared radiation ceramic material (size 3 mm. times.4 mm. times.36 mm) had a bending strength of 73MPa as measured by a three-point bending method. The density of the silicon carbide infrared radiation ceramic material measured by an Archimedes drainage method is 2.03g/cm3

Claims (10)

1. The silicon carbide infrared radiation ceramic material is characterized by comprising the following raw materials: 76.5 to 95wt% of beta-SiC, 0 to 8.5wt% of AlN, and MgO-Al in an amount of not 0 but 5 to 15wt%2O3-SiO2The additive accounts for 100wt% of the total content of the components;
the MgO-Al2O3-SiO2The auxiliary agent comprises the following raw material components: 10 to 30wt% of MgO and 15 to 40wt% of Al2O3、20~60wt% SiO2The sum of the contents of all the components is 100 wt%;
the preparation method of the silicon carbide infrared radiation ceramic material comprises the following steps:
(1) selecting beta-SiC powder and AlN powder as raw material powder, mixing, and carrying out solid solution reaction at 1700-2000 ℃ to obtain solid solution powder;
(2) mixing the obtained solid solution powder with MgO-Al2O3-SiO2Mixing the auxiliary agents to obtain mixed powder;
(3) pressing and molding the obtained mixed powder, and then performing vacuum de-bonding and sintering to obtain the silicon carbide infrared radiation ceramic material;
the silicon carbide infrared radiation ceramic material has an infrared emissivity of 0.75-0.84 at a normal temperature of 2.5-16 mu m.
2. The silicon carbide infrared radiation ceramic material as claimed in claim 1, wherein the density of the silicon carbide infrared radiation ceramic material is 2.01-2.50 g/cm3The bending strength is 68-210 MPa.
3. Silicon carbide infrared radiating ceramic material according to claim 1, characterised in that it is MgO-Al in terms of its properties2O3-SiO2Raw material components of the auxiliary agent are weighed MgO powder and Al2O3Powder and SiO2Mixing the powder to obtain the MgO-Al2O3-SiO2And (4) an auxiliary agent.
4. The silicon carbide infrared radiation ceramic material of claim 3, wherein the particle size of the beta-SiC powder is 0.5 to 1 μm; the particle size of the AlN powder is 1-2 mu m; the particle size of the MgO powder is 1-3 μm; the Al is2O3The particle size of the powder is 100-200 nm; the SiO2The particle size of the powder is 1 to 3 μm.
5. The silicon carbide infrared radiating ceramic material of claim 1, wherein the atmosphere of the solution reaction is an inert atmosphere; the gas pressure of the solid solution reaction is 40-75 mbar; the time of the solid solution reaction is 2-4 hours.
6. The silicon carbide infrared radiating ceramic material of claim 5, wherein the atmosphere of the solid solution reaction is an argon atmosphere.
7. The silicon carbide infrared radiation ceramic material as claimed in claim 1, wherein the raw material powder or mixed powder further comprises a binder; the binder is selected from at least one of phenolic resin, polyvinyl alcohol PVA and polyvinyl butyral PVB; the addition amount of the binder is not more than 8wt% of the total mass of the raw material powder or the mixed powder.
8. The silicon carbide infrared radiation ceramic material as claimed in claim 1, wherein the temperature of the vacuum de-bonding is 700 ℃ to 1000 ℃, the time is 0.5 to 2 hours, and the vacuum degree is-5 to 10 Pa.
9. The silicon carbide infrared radiating ceramic material of claim 1, wherein the sintering atmosphere is an inert atmosphere; the pressure of the inert atmosphere is 40-75 mbar; the sintering temperature is 1400-1950 ℃; the sintering time is 1-3 hours.
10. The silicon carbide infrared radiating ceramic material of claim 9, wherein the sintering atmosphere is an argon atmosphere.
CN202010061183.3A 2020-01-19 2020-01-19 Silicon carbide infrared radiation ceramic material and preparation method thereof Active CN111170743B (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CN202010061183.3A CN111170743B (en) 2020-01-19 2020-01-19 Silicon carbide infrared radiation ceramic material and preparation method thereof

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
CN202010061183.3A CN111170743B (en) 2020-01-19 2020-01-19 Silicon carbide infrared radiation ceramic material and preparation method thereof

Publications (2)

Publication Number Publication Date
CN111170743A CN111170743A (en) 2020-05-19
CN111170743B true CN111170743B (en) 2021-08-31

Family

ID=70651116

Family Applications (1)

Application Number Title Priority Date Filing Date
CN202010061183.3A Active CN111170743B (en) 2020-01-19 2020-01-19 Silicon carbide infrared radiation ceramic material and preparation method thereof

Country Status (1)

Country Link
CN (1) CN111170743B (en)

Families Citing this family (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113788685A (en) * 2021-09-08 2021-12-14 中国科学院上海硅酸盐研究所 Low-temperature sintered cordierite/silicon carbide composite ceramic solar thermal power generation heat-absorbing body material and preparation method thereof
CN116675538B (en) * 2023-05-30 2023-12-22 中国科学院上海硅酸盐研究所 Method for preparing SiC ceramic by combining selective laser 3D printing/precursor dipping pyrolysis/liquid phase sintering

Family Cites Families (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1331560C (en) * 2004-10-13 2007-08-15 中国科学院上海硅酸盐研究所 Low temperature sintering reticular silicon carbide ceramic filtering device with high fire resisting level and its preparation method
CN1800097A (en) * 2006-01-18 2006-07-12 中国科学院上海硅酸盐研究所 Silicon carbide-cordierite composite porous ceramic and its preparation method
CN104072142A (en) * 2014-06-30 2014-10-01 江苏新光环保工程有限公司 Preparation method of oxide combined SiC porous ceramic
CN106278277B (en) * 2016-08-21 2019-05-24 南京洛普科技有限公司 A kind of sharp cone distal silicon carbide ceramics absorber and preparation method thereof
CN110078514B (en) * 2019-05-23 2021-08-31 中国科学院上海硅酸盐研究所 Silicon carbide ceramic microwave calibration source

Also Published As

Publication number Publication date
CN111170743A (en) 2020-05-19

Similar Documents

Publication Publication Date Title
CN106588021B (en) A kind of silicon carbide ceramics and preparation method thereof
JP4812144B2 (en) Aluminum nitride sintered body and manufacturing method thereof
CN111170743B (en) Silicon carbide infrared radiation ceramic material and preparation method thereof
CN110483060B (en) High-thermal-conductivity silicon nitride ceramic and preparation method thereof
EP0743290B1 (en) Aluminum nitride sinter and production method therefor
CN101734923A (en) Aluminum nitride porous ceramic and preparation method thereof
CN107365155B (en) Low-temperature sintering aid system of aluminum nitride ceramic
CN110937893A (en) Method for improving energy density of pyroelectric composite ceramic material
CN113943162A (en) alpha-SiAlON high-entropy transparent ceramic material and preparation method thereof
CN108863395B (en) High-thermal-conductivity and high-strength silicon nitride ceramic material and preparation method thereof
CN110423122B (en) Preparation method of low-loss and high-thermal-conductivity silicon nitride ceramic
CN109704780B (en) Thermal shock resistant boron nitride-strontium feldspar ceramic matrix composite material and preparation method thereof
CN110937898B (en) Preparation method of sesquioxide window material
JP4410479B2 (en) Electromagnetic wave absorber
CN1254454C (en) Cylon-corundum powdery material and its production
CN109650862B (en) High-temperature-resistant boron nitride-strontium feldspar ceramic matrix composite material and preparation method thereof
CN111410537B (en) Boron carbide-based complex phase ceramic material with linear conductive characteristic and preparation method thereof
JP5031541B2 (en) Silicon nitride sintered body, circuit board, and power semiconductor module
JP3756345B2 (en) Aluminum nitride-based sintered body, method for producing the same, and susceptor using the same
WO1998032711A1 (en) Gas pressure sintered silicon nitride having high strength and stress rupture resistance
CN109320263B (en) Sintering aid, quartz ceramic, and preparation and application methods thereof
US20120211485A1 (en) Heat insulation material for microwave heating and method for manufacturing the same
KR20210088361A (en) Method for Preparing Silicon Nitride Sintered Body and The Silicon Nitride Sintered Body Prepared by The Same
CN109734453B (en) Boron nitride-strontium feldspar ceramic matrix composite material for aerospace heat protection and preparation method thereof
KR20200052841A (en) MoCu HEAT DISSIPATION MATERIAL WITH CARBON PARTICLES AND PREPARING METHOD THEREOF

Legal Events

Date Code Title Description
PB01 Publication
PB01 Publication
SE01 Entry into force of request for substantive examination
SE01 Entry into force of request for substantive examination
GR01 Patent grant
GR01 Patent grant