CN112898031A - High-thermal-conductivity high-toughness silicon nitride ceramic material containing rare earth elements and preparation method thereof - Google Patents
High-thermal-conductivity high-toughness silicon nitride ceramic material containing rare earth elements and preparation method thereof Download PDFInfo
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- 229910052581 Si3N4 Inorganic materials 0.000 title claims abstract description 56
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 title claims abstract description 52
- 229910010293 ceramic material Inorganic materials 0.000 title claims abstract description 37
- 229910052761 rare earth metal Inorganic materials 0.000 title claims abstract description 34
- 238000002360 preparation method Methods 0.000 title abstract description 8
- 239000000843 powder Substances 0.000 claims abstract description 46
- 238000005245 sintering Methods 0.000 claims abstract description 35
- 239000002131 composite material Substances 0.000 claims abstract description 32
- 150000002910 rare earth metals Chemical class 0.000 claims abstract description 18
- 229910001404 rare earth metal oxide Inorganic materials 0.000 claims abstract description 16
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 10
- 239000001301 oxygen Substances 0.000 claims abstract description 10
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 10
- 239000003638 chemical reducing agent Substances 0.000 claims abstract description 6
- 239000002245 particle Substances 0.000 claims description 11
- 238000000034 method Methods 0.000 claims description 10
- 238000000498 ball milling Methods 0.000 claims description 9
- 239000012298 atmosphere Substances 0.000 claims description 6
- 238000002156 mixing Methods 0.000 claims description 6
- 230000001681 protective effect Effects 0.000 claims description 6
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 4
- 238000001035 drying Methods 0.000 claims description 4
- 238000007873 sieving Methods 0.000 claims description 4
- 238000010146 3D printing Methods 0.000 claims description 2
- 229910052684 Cerium Inorganic materials 0.000 claims description 2
- 229910052692 Dysprosium Inorganic materials 0.000 claims description 2
- 229910052691 Erbium Inorganic materials 0.000 claims description 2
- 229910052693 Europium Inorganic materials 0.000 claims description 2
- 229910052688 Gadolinium Inorganic materials 0.000 claims description 2
- 229910052689 Holmium Inorganic materials 0.000 claims description 2
- 229910052765 Lutetium Inorganic materials 0.000 claims description 2
- 229910052779 Neodymium Inorganic materials 0.000 claims description 2
- 229910052777 Praseodymium Inorganic materials 0.000 claims description 2
- 229910052772 Samarium Inorganic materials 0.000 claims description 2
- 229910052771 Terbium Inorganic materials 0.000 claims description 2
- 229910052775 Thulium Inorganic materials 0.000 claims description 2
- 229910052769 Ytterbium Inorganic materials 0.000 claims description 2
- 229910052786 argon Inorganic materials 0.000 claims description 2
- 238000005266 casting Methods 0.000 claims description 2
- 229910000421 cerium(III) oxide Inorganic materials 0.000 claims description 2
- 238000009694 cold isostatic pressing Methods 0.000 claims description 2
- NLQFUUYNQFMIJW-UHFFFAOYSA-N dysprosium(III) oxide Inorganic materials O=[Dy]O[Dy]=O NLQFUUYNQFMIJW-UHFFFAOYSA-N 0.000 claims description 2
- VQCBHWLJZDBHOS-UHFFFAOYSA-N erbium(III) oxide Inorganic materials O=[Er]O[Er]=O VQCBHWLJZDBHOS-UHFFFAOYSA-N 0.000 claims description 2
- RSEIMSPAXMNYFJ-UHFFFAOYSA-N europium(III) oxide Inorganic materials O=[Eu]O[Eu]=O RSEIMSPAXMNYFJ-UHFFFAOYSA-N 0.000 claims description 2
- CMIHHWBVHJVIGI-UHFFFAOYSA-N gadolinium(III) oxide Inorganic materials [O-2].[O-2].[O-2].[Gd+3].[Gd+3] CMIHHWBVHJVIGI-UHFFFAOYSA-N 0.000 claims description 2
- JYTUFVYWTIKZGR-UHFFFAOYSA-N holmium oxide Inorganic materials [O][Ho]O[Ho][O] JYTUFVYWTIKZGR-UHFFFAOYSA-N 0.000 claims description 2
- 238000001513 hot isostatic pressing Methods 0.000 claims description 2
- 238000007731 hot pressing Methods 0.000 claims description 2
- 229910052746 lanthanum Inorganic materials 0.000 claims description 2
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum oxide Inorganic materials [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 claims description 2
- 229910003443 lutetium oxide Inorganic materials 0.000 claims description 2
- PLDDOISOJJCEMH-UHFFFAOYSA-N neodymium oxide Inorganic materials [O-2].[O-2].[O-2].[Nd+3].[Nd+3] PLDDOISOJJCEMH-UHFFFAOYSA-N 0.000 claims description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N nitrogen Substances N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 2
- 229910052757 nitrogen Inorganic materials 0.000 claims description 2
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 claims description 2
- KTUFCUMIWABKDW-UHFFFAOYSA-N oxo(oxolanthaniooxy)lanthanum Chemical compound O=[La]O[La]=O KTUFCUMIWABKDW-UHFFFAOYSA-N 0.000 claims description 2
- 238000003825 pressing Methods 0.000 claims description 2
- FKTOIHSPIPYAPE-UHFFFAOYSA-N samarium(III) oxide Inorganic materials [O-2].[O-2].[O-2].[Sm+3].[Sm+3] FKTOIHSPIPYAPE-UHFFFAOYSA-N 0.000 claims description 2
- 229910052706 scandium Inorganic materials 0.000 claims description 2
- HYXGAEYDKFCVMU-UHFFFAOYSA-N scandium(III) oxide Inorganic materials O=[Sc]O[Sc]=O HYXGAEYDKFCVMU-UHFFFAOYSA-N 0.000 claims description 2
- ZIKATJAYWZUJPY-UHFFFAOYSA-N thulium (III) oxide Inorganic materials [O-2].[O-2].[O-2].[Tm+3].[Tm+3] ZIKATJAYWZUJPY-UHFFFAOYSA-N 0.000 claims description 2
- FIXNOXLJNSSSLJ-UHFFFAOYSA-N ytterbium(III) oxide Inorganic materials O=[Yb]O[Yb]=O FIXNOXLJNSSSLJ-UHFFFAOYSA-N 0.000 claims description 2
- 229910052727 yttrium Inorganic materials 0.000 claims description 2
- 238000010345 tape casting Methods 0.000 claims 1
- 239000012535 impurity Substances 0.000 abstract description 2
- 239000012299 nitrogen atmosphere Substances 0.000 description 8
- 239000000919 ceramic Substances 0.000 description 6
- 230000017525 heat dissipation Effects 0.000 description 6
- 239000011812 mixed powder Substances 0.000 description 6
- 239000000758 substrate Substances 0.000 description 6
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 4
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 4
- 229910002804 graphite Inorganic materials 0.000 description 4
- 239000010439 graphite Substances 0.000 description 4
- 238000000227 grinding Methods 0.000 description 4
- 238000010438 heat treatment Methods 0.000 description 4
- 239000002002 slurry Substances 0.000 description 4
- 239000000463 material Substances 0.000 description 3
- 239000013078 crystal Substances 0.000 description 2
- 238000009413 insulation Methods 0.000 description 2
- 238000000465 moulding Methods 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 238000005452 bending Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- PMHQVHHXPFUNSP-UHFFFAOYSA-M copper(1+);methylsulfanylmethane;bromide Chemical compound Br[Cu].CSC PMHQVHHXPFUNSP-UHFFFAOYSA-M 0.000 description 1
- 229910003460 diamond Inorganic materials 0.000 description 1
- 239000010432 diamond Substances 0.000 description 1
- 238000005530 etching Methods 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 238000001746 injection moulding Methods 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- 238000011056 performance test Methods 0.000 description 1
- 238000013001 point bending Methods 0.000 description 1
- 230000035939 shock Effects 0.000 description 1
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 1
- 229910010271 silicon carbide Inorganic materials 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
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- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/515—Shaped 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
- C04B35/58—Shaped 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 borides, nitrides, i.e. nitrides, oxynitrides, carbonitrides or oxycarbonitrides or silicides
- C04B35/584—Shaped 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 borides, nitrides, i.e. nitrides, oxynitrides, carbonitrides or oxycarbonitrides or silicides based on silicon nitride
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Abstract
The invention relates to the technical field of ceramic materials, in particular to a silicon nitride ceramic material containing rare earth elements and having high thermal conductivity and high toughness and a preparation method of the silicon nitride ceramic material. According to the invention, rare earth metal is added to replace part of rare earth oxide in the composite powder, and the rare earth metal is used as an oxygen reducer, so that oxygen element introduced by a sintering aid can be reduced and oxygen impurities in the silicon nitride powder are captured, thereby obviously improving the sintering behavior, improving the thermal conductivity, strength and fracture toughness of the silicon nitride, and preparing the high-thermal-conductivity and high-toughness silicon nitride ceramic material.
Description
Technical Field
The invention relates to the technical field of ceramic materials, in particular to a high-thermal-conductivity and high-toughness silicon nitride ceramic material containing rare earth elements and a preparation method of the silicon nitride ceramic material.
Background
With the application of high-power electronic components represented by electric vehicles, such as an alternating current-direct current conversion module, not only is the power increased and the required heat dissipation capacity increased, but also the working environment has serious shock impact conditions, the required strength is higher, and good dielectric properties are required under high-strength alternating current. At present, in a ceramic insulating heat dissipation substrate, an aluminum oxide heat dissipation substrate with low cost has low heat conductivity, is commonly used for a module with low power, an aluminum nitride heat dissipation substrate with high heat conductivity has low strength, is commonly used for a module with high power, a silicon carbide heat dissipation substrate with high strength and high heat conductivity has poor insulation, and a silicon nitride heat dissipation substrate is widely researched by virtue of the advantages of high strength, high fracture toughness, high insulation, heat conductivity meeting requirements and the like. The silicon nitride ceramic material has high preparation cost, the silicon nitride ceramic material with high thermal conductivity is generally prepared by a long-time, high-temperature and high-pressure method, when one performance of the existing silicon nitride ceramic is improved, other performance is generally sacrificed, and the mechanical performance of the silicon nitride ceramic prepared by the long-time, high-temperature and high-pressure method is reduced and the cost is very high.
Disclosure of Invention
Aiming at the problems in the prior art, the invention provides a silicon nitride substrate ceramic material containing rare earth elements, which has high thermal conductivity and high toughness, and a preparation method thereof.
In order to achieve the purpose, the invention adopts the following technical scheme.
The invention provides a high-heat-conductivity high-toughness silicon nitride ceramic material containing rare earth elements, which is formed by sintering composite powder, wherein the composite powder comprises silicon nitride powder and an oxygen reducing agent; the oxygen reducing agent is rare earth metal.
Preferably, the particle size of the silicon nitride powder is 10 nm-20 μm; more preferably, the particle size of the silicon nitride powder is 200nm to 1 μm.
Preferably, the rare earth metal is selected from one or more of Yb, Lu, Sc, Y, La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er and Tm.
Preferably, the particle size of the rare earth metal is 100 μm or less, and more preferably, the particle size of the rare earth metal is 25 μm or less.
Preferably, the content of the rare earth metal in the composite powder is less than or equal to 15 wt%; more preferably, the content of the rare earth metal in the composite powder is 0.5 wt% to 6 wt%.
Preferably, the composite powder further comprises a rare earth oxide.
Preferably, the rare earth oxide is selected from Yb2O3、Lu2O3、Sc2O3、Y2O3、La2O3、Ce2O3、Pr2O3、Nd2O3、Pm2O3、Sm2O3、Eu2O3、Gd2O3、Tb2O3、Dy2O3、Ho2O3、Er2O3And Tm2O3One or more of (a).
Preferably, the particle size of the rare earth oxide is 10 nm-20 μm; more preferably, the particle size of the rare earth oxide is 40nm to 1 μm.
Preferably, the content of the rare earth oxide in the composite powder is less than or equal to 15 wt%; more preferably, the content of the rare earth oxide in the composite powder is 0.5 wt% to 5 wt%.
In another aspect of the present invention, a method for preparing the above high thermal conductivity and high toughness silicon nitride ceramic material containing rare earth elements is provided, which comprises the following steps:
uniformly mixing all components for forming the composite powder to obtain the composite powder; molding the composite powder to obtain a blank; performing primary sintering and secondary sintering on the green body; the first sintering is carried out for 0.5-4 hours at 800-1700 ℃ under the protective atmosphere of 0-10 MPa, and the second sintering is carried out for 1-6 hours at 1700-1900 ℃ under the protective atmosphere of 0.1-10 MPa.
Preferably, the components for forming the composite powder are subjected to ball milling, drying, crushing and sieving processes to obtain the uniformly mixed composite powder.
Preferably, the forming comprises dry pressing, cold isostatic pressing, casting, gel injection molding or 3D printing. The method of molding is not limited to these.
Preferably, the sintering includes pressureless hot-pressing sintering, air-pressure sintering or hot isostatic pressing sintering. The method of sintering is not limited to these.
The protective atmosphere is nitrogen or argon, etc.
Compared with the prior art, the invention has the beneficial effects that:
according to the invention, the rare earth metal is added to replace all or part of rare earth oxide in the composite powder, and the rare earth metal is used as an oxygen reducer, so that oxygen element introduced by a sintering aid can be reduced and oxygen impurities in the silicon nitride powder are captured, thereby obviously improving the sintering behavior, improving the thermal conductivity, strength and fracture toughness of the silicon nitride, and preparing the high-thermal-conductivity and high-toughness silicon nitride ceramic material.
Detailed Description
In order to more fully understand the technical contents of the present invention, the technical solutions of the present invention will be further described and illustrated with reference to the following specific embodiments.
The silicon nitride powder used in the following examples had a particle size of 0.2 μm, the rare earth oxide had a particle size of 0.5 μm, and the rare earth metal was used after passing through a 500-mesh sieve, and the particle size of the rare earth metal was 25 μm or less.
Example 1
The embodiment provides a silicon nitride ceramic material with high thermal conductivity and high toughness and a preparation method thereof, and the preparation method specifically comprises the following steps: mixing 95 g of Si3N4And 5 g of Y2O3Adding into absolute ethyl alcohol to prepare mixed powder, adding into grinding balls with a ball-material ratio of 1: 3, ball-milling for 10 hours, putting the ball-milled slurry into a rotary evaporator, heating to 60 ℃, drying the powder, and sieving with a 100-mesh sieve to obtain the composite powder. And (2) putting a proper amount of the uniformly mixed composite powder into a graphite die with the diameter of 50mm for sintering, carrying out hot-press sintering at 1600 ℃, 0.1MPa of nitrogen atmosphere and 30MPa of unidirectional pressure for 1 hour, and then carrying out hot-press sintering at 1850 ℃, 0.1MPa of nitrogen atmosphere and 30MPa of unidirectional pressure for 3 hours to prepare the silicon nitride ceramic material.
Example 2
Mixing 95 g of Si3N43 g of Y2O3And 2 g of Y are added into absolute ethyl alcohol to prepare mixed powder, grinding balls are placed into the mixed powder, the ball-material ratio is 1: 3, after ball milling is carried out for 10 hours, the slurry after ball milling is placed into a rotary evaporator, the heating temperature is 60 ℃, after the powder is dried, the powder is sieved by a 100-mesh sieve, and the composite powder is obtained. Get fitAnd (3) putting the uniformly mixed composite powder into a graphite die with the diameter of 50mm for sintering, carrying out hot-press sintering at 1600 ℃, 0.1MPa of nitrogen atmosphere and 30MPa of unidirectional pressure for 1 hour, and then carrying out hot-press sintering at 1850 ℃, 0.1MPa of nitrogen atmosphere and 30MPa of unidirectional pressure for 3 hours to prepare the high-thermal-conductivity and high-toughness silicon nitride ceramic material.
Example 3
Mixing 96 g of Si3N42 g of Y2O3And 2 g of Y are added into absolute ethyl alcohol to prepare mixed powder, grinding balls are placed into the mixed powder, the ball-material ratio is 1: 3, after ball milling is carried out for 10 hours, the slurry after ball milling is placed into a rotary evaporator, the heating temperature is 60 ℃, after the powder is dried, the powder is sieved by a 100-mesh sieve, and the composite powder is obtained. And (2) putting a proper amount of uniformly mixed composite powder into a graphite die with the diameter of 50mm for sintering, carrying out hot-press sintering at 1600 ℃, 0.1MPa of nitrogen atmosphere and 30MPa of unidirectional pressure for 1 hour, and then carrying out hot-press sintering at 1850 ℃, 0.1MPa of nitrogen atmosphere and 30MPa of unidirectional pressure for 3 hours to prepare the high-thermal-conductivity and high-toughness silicon nitride ceramic material.
Example 4
Mixing 96 g of Si3N4Adding 4 g of Y into absolute ethyl alcohol to prepare mixed powder, adding grinding balls, carrying out ball milling for 10 hours, adding the slurry after ball milling into a rotary evaporator, heating to 60 ℃, drying the powder, and sieving with a 100-mesh sieve to obtain the composite powder. And (2) putting a proper amount of uniformly mixed composite powder into a graphite die with the diameter of 50mm for sintering, carrying out hot-press sintering at 1600 ℃, 0.1MPa of nitrogen atmosphere and 30MPa of unidirectional pressure for 1 hour, and then carrying out hot-press sintering at 1850 ℃, 0.1MPa of nitrogen atmosphere and 30MPa of unidirectional pressure for 3 hours to prepare the high-thermal-conductivity and high-toughness silicon nitride ceramic material.
The silicon nitride ceramic materials obtained in examples 1-4 were processed, and the sample made from the silicon nitride ceramic material of example 1 was numbered 1, and the samples made from the silicon nitride ceramic materials of examples 2-4 were correspondingly numbered 2-4.
The silicon nitride ceramic materials prepared in the examples were processed by a diamond tool, and a plurality of 1mm × 2mm × 25mm sample strips and a plurality of 10mm × 10mm × 2mm sample blocks were prepared from the silicon nitride ceramic materials of the examples, respectively, and were used for testing three-point bending strength and thermal conductivity of the silicon nitride ceramic materials. Relative density was measured using archimedes' method. In addition, phase identification was performed by X-ray diffraction, and the obtained silicon nitride ceramic material after the polish-etching treatment was observed by a scanning electron microscope.
TABLE 1 results of performance test of silicon nitride ceramics prepared in each example
| Density g/cm3 | Bending strength MPa | Thermal conductivity W/mK | |
| Number 1 | 3.21 | 770 | 47 |
| Number 2 | 3.24 | 807 | 63 |
| No. 3 | 3.23 | 770 | 60 |
| Number 4 | 3.22 | 728 | 59 |
The test results in table 1 show that the silicon nitride ceramics added with rare earth metals are compact and have high thermal conductivity, and excellent mechanical properties are ensured under a proper rare earth oxide proportion. Under the condition of proper proportion of rare earth metal and rare earth oxide, XRD detects second phase crystal phase, and under the condition of scanning electron microscope it observes the microstructure of glass phase aggregated to trifurcate grain boundary formed by silicon nitride crystal grain, so that it can obtain high-thermal conductivity and high-toughness silicon nitride ceramic.
The technical contents of the present invention are further illustrated by the examples, so as to facilitate the understanding of the reader, but the embodiments of the present invention are not limited thereto, and any technical extension or re-creation based on the present invention is protected by the present invention.
Claims (10)
1. A silicon nitride ceramic material containing rare earth elements and having high heat conductivity and high toughness is prepared by sintering composite powder, and is characterized in that: the composite powder comprises silicon nitride powder and an oxygen reducing agent; the oxygen reducing agent is rare earth metal.
2. The high-thermal-conductivity high-toughness silicon nitride ceramic material containing rare earth elements as claimed in claim 1, wherein: the composite powder also comprises rare earth oxide.
3. The high thermal conductivity high toughness silicon nitride ceramic material containing rare earth elements as claimed in claim 1 or 2, wherein: the rare earth metal is selected from one or more of Yb, Lu, Sc, Y, La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er and Tm.
4. The high-thermal-conductivity high-toughness silicon nitride ceramic material containing rare earth elements as claimed in claim 3, wherein: the particle size of the rare earth metal is less than 100 mu m.
5. The high thermal conductivity high toughness silicon nitride ceramic material containing rare earth elements as claimed in claim 1 or 2, wherein: the content of rare earth metal in the composite powder is less than or equal to 15 wt%.
6. The high-heat-conductivity high-toughness silicon nitride ceramic material containing rare earth elements as claimed in claim 2, wherein: said rare earth oxide is selected from Yb2O3、Lu2O3、Sc2O3、Y2O3、La2O3、Ce2O3、Pr2O3、Nd2O3、Pm2O3、Sm2O3、Eu2O3、Gd2O3、Tb2O3、Dy2O3、Ho2O3、Er2O3And Tm2O3One or more of (a).
7. The high-thermal-conductivity high-toughness silicon nitride ceramic material containing rare earth elements as claimed in claim 6, wherein: the content of the rare earth oxide in the composite powder is less than or equal to 15 wt%.
8. The high-thermal-conductivity high-toughness silicon nitride ceramic material containing rare earth elements as claimed in claim 6, wherein: the particle size of the rare earth oxide is 10 nm-20 mu m; the grain diameter of the silicon nitride powder is 10 nm-20 mu m.
9. A method for preparing a high-thermal-conductivity high-toughness silicon nitride ceramic material containing rare earth elements as claimed in claim 1, which comprises the following steps:
s1, uniformly mixing all the components for forming the composite powder to obtain the composite powder;
s2, forming the composite powder to obtain a blank;
s3, sintering the blank for the first time, wherein the first sintering is carried out for 0.5-4 hours at 800-1700 ℃ under the protective atmosphere of 0-10 MPa;
and S4, sintering the blank for the second time, wherein the sintering for the second time is carried out for 1-6 hours at 1700-1900 ℃ under the protective atmosphere of 0.1-10 MPa.
10. The method for preparing the high-thermal-conductivity high-toughness silicon nitride ceramic material containing the rare earth elements as claimed in claim 9, is characterized in that:
the components for forming the composite powder are subjected to ball milling, drying, crushing and sieving processes to obtain uniformly mixed composite powder;
the sintering comprises pressureless hot-pressing sintering, air pressure sintering or hot isostatic pressing sintering;
the forming comprises dry pressing forming, cold isostatic pressing forming, tape casting forming, gel casting forming or 3D printing forming;
the protective atmosphere is nitrogen or argon.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2023024273A1 (en) * | 2021-08-27 | 2023-03-02 | 广东工业大学 | Non-oxide y3si2c2 sintering aid, high-performance silicon nitride ceramic substrate, and preparation methods therefor |
| CN116239387A (en) * | 2023-02-09 | 2023-06-09 | 中国科学院金属研究所 | Preparation method of high-strength silicon nitride by using medium/high entropy multi-element rare earth sintering aid |
Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5132257A (en) * | 1987-03-16 | 1992-07-21 | Hitachi, Ltd. | Composite ceramic sintered body and process for production thereof |
| CN101100388A (en) * | 2007-07-17 | 2008-01-09 | 清华大学 | High heat conductivity silicon nitride ceramics material and preparation method thereof |
| CN107434416A (en) * | 2017-08-02 | 2017-12-05 | 上海海事大学 | A kind of high tough silicon nitride ceramic material and its sintering aid and sintering method |
| CN109627014A (en) * | 2019-01-14 | 2019-04-16 | 中国科学院上海硅酸盐研究所 | A kind of high-intensitive, high-termal conductivity Si3N4Ceramic material and preparation method thereof |
-
2019
- 2019-11-19 CN CN201911138740.0A patent/CN112898031A/en active Pending
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5132257A (en) * | 1987-03-16 | 1992-07-21 | Hitachi, Ltd. | Composite ceramic sintered body and process for production thereof |
| CN101100388A (en) * | 2007-07-17 | 2008-01-09 | 清华大学 | High heat conductivity silicon nitride ceramics material and preparation method thereof |
| CN107434416A (en) * | 2017-08-02 | 2017-12-05 | 上海海事大学 | A kind of high tough silicon nitride ceramic material and its sintering aid and sintering method |
| CN109627014A (en) * | 2019-01-14 | 2019-04-16 | 中国科学院上海硅酸盐研究所 | A kind of high-intensitive, high-termal conductivity Si3N4Ceramic material and preparation method thereof |
Non-Patent Citations (1)
| Title |
|---|
| 李懋强: "《热学陶瓷——性能 测试 工艺》", 30 June 2013, 中国建材工业出版社 * |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2023024273A1 (en) * | 2021-08-27 | 2023-03-02 | 广东工业大学 | Non-oxide y3si2c2 sintering aid, high-performance silicon nitride ceramic substrate, and preparation methods therefor |
| CN116239387A (en) * | 2023-02-09 | 2023-06-09 | 中国科学院金属研究所 | Preparation method of high-strength silicon nitride by using medium/high entropy multi-element rare earth sintering aid |
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