CN116425551A - Low-temperature sintering process of aluminum nitride ceramic material - Google Patents
Low-temperature sintering process of aluminum nitride ceramic material Download PDFInfo
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- PMHQVHHXPFUNSP-UHFFFAOYSA-M copper(1+);methylsulfanylmethane;bromide Chemical compound Br[Cu].CSC PMHQVHHXPFUNSP-UHFFFAOYSA-M 0.000 title claims abstract description 62
- 229910010293 ceramic material Inorganic materials 0.000 title claims abstract description 39
- 238000000034 method Methods 0.000 title claims abstract description 26
- 230000008569 process Effects 0.000 title claims abstract description 21
- 238000009766 low-temperature sintering Methods 0.000 title claims abstract description 18
- 238000005245 sintering Methods 0.000 claims abstract description 38
- 239000002113 nanodiamond Substances 0.000 claims abstract description 32
- 239000000843 powder Substances 0.000 claims abstract description 25
- 239000011812 mixed powder Substances 0.000 claims abstract description 24
- 238000007731 hot pressing Methods 0.000 claims abstract description 19
- 238000000498 ball milling Methods 0.000 claims abstract description 15
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims abstract description 12
- 238000002156 mixing Methods 0.000 claims abstract description 11
- 238000001035 drying Methods 0.000 claims abstract description 10
- 229910052751 metal Inorganic materials 0.000 claims abstract description 8
- 239000002184 metal Substances 0.000 claims abstract description 8
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 7
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 6
- 229910002804 graphite Inorganic materials 0.000 claims abstract description 6
- 239000010439 graphite Substances 0.000 claims abstract description 6
- 238000000227 grinding Methods 0.000 claims abstract description 6
- 229910052757 nitrogen Inorganic materials 0.000 claims abstract description 6
- 238000007873 sieving Methods 0.000 claims abstract description 6
- 238000005056 compaction Methods 0.000 claims abstract description 3
- 239000002253 acid Substances 0.000 claims description 9
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 5
- 238000001354 calcination Methods 0.000 claims description 5
- 229910017604 nitric acid Inorganic materials 0.000 claims description 5
- QAOWNCQODCNURD-UHFFFAOYSA-N sulfuric acid Substances OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims description 5
- 238000003756 stirring Methods 0.000 claims description 4
- 238000005406 washing Methods 0.000 claims description 4
- 230000004048 modification Effects 0.000 claims description 3
- 238000012986 modification Methods 0.000 claims description 3
- 229910003460 diamond Inorganic materials 0.000 claims description 2
- 239000010432 diamond Substances 0.000 claims description 2
- 229910018068 Li 2 O Inorganic materials 0.000 claims 1
- 239000012752 auxiliary agent Substances 0.000 abstract description 4
- 230000000052 comparative effect Effects 0.000 description 11
- 239000013078 crystal Substances 0.000 description 8
- 239000000919 ceramic Substances 0.000 description 5
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 4
- 229910003481 amorphous carbon Inorganic materials 0.000 description 4
- 239000007791 liquid phase Substances 0.000 description 4
- 230000007935 neutral effect Effects 0.000 description 4
- 229910052760 oxygen Inorganic materials 0.000 description 4
- 230000009471 action Effects 0.000 description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 239000001301 oxygen Substances 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
- 238000001291 vacuum drying Methods 0.000 description 3
- JQMFQLVAJGZSQS-UHFFFAOYSA-N 2-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperazin-1-yl]-N-(2-oxo-3H-1,3-benzoxazol-6-yl)acetamide Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)N1CCN(CC1)CC(=O)NC1=CC2=C(NC(O2)=O)C=C1 JQMFQLVAJGZSQS-UHFFFAOYSA-N 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 125000004430 oxygen atom Chemical group O* 0.000 description 2
- 230000002195 synergetic effect Effects 0.000 description 2
- 238000005054 agglomeration Methods 0.000 description 1
- 230000002776 aggregation Effects 0.000 description 1
- 230000004075 alteration Effects 0.000 description 1
- 150000004645 aluminates Chemical class 0.000 description 1
- JNDMLEXHDPKVFC-UHFFFAOYSA-N aluminum;oxygen(2-);yttrium(3+) Chemical compound [O-2].[O-2].[O-2].[Al+3].[Y+3] JNDMLEXHDPKVFC-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000000280 densification Methods 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 238000010292 electrical insulation Methods 0.000 description 1
- 230000020477 pH reduction Effects 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
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Abstract
The invention discloses a low-temperature sintering process of an aluminum nitride ceramic material, which belongs to the technical field of ceramic materials and comprises the following steps: s1, mixing aluminum nitride powder, nano diamond and a sintering aid to obtain mixed powder; s2, adding the mixed powder, absolute ethyl alcohol and a ball milling medium into a ball mill according to a mass ratio of 1:1:5-6, and drying, grinding and sieving after ball milling and dispersing uniformly to obtain sintered powder; s3, adding the sintered powder into a hot-pressing metal mold for compaction to obtain a blank; s4, transferring the blank into a graphite mold, and carrying out low-temperature hot-pressing sintering for 2-3 hours under the conditions of the temperature of 1600-1650 ℃ and the pressure of 25-30MPa and nitrogen protection to obtain an aluminum nitride ceramic material; according to the invention, the nano diamond and the multi-element sintering auxiliary agent are matched for use, so that the sintering temperature can be reduced, and the aluminum nitride ceramic material with high density, high heat conductivity and strong fracture toughness is obtained.
Description
Technical Field
The invention belongs to the technical field of ceramic materials, and particularly relates to a low-temperature sintering process of an aluminum nitride ceramic material.
Background
Aluminum nitride ceramics are considered as a very promising ceramic material because of their excellent characteristics such as high thermal conductivity, excellent electrical insulation and dielectric properties, good flexural strength and hardness, strong corrosion resistance, a coefficient of thermal expansion matching with silicon, and the like, and have been widely used in recent years. Aluminum nitride belongs to a covalent compound, the self-diffusion coefficient is small, the direct sintering densification of the aluminum nitride is difficult, the theoretical thermal conductivity of the aluminum nitride ceramic is as high as 320W/(m.K), but the thermal conductivity of the actually produced aluminum nitride ceramic is far from the theoretical value, so that the sintering auxiliary agent is usually added to promote the sintering in the preparation of the aluminum nitride ceramic at present, and even if the sintering auxiliary agent is added to prepare the aluminum nitride ceramic, the sintering process still needs a high temperature of more than 1800 ℃ to obtain the aluminum nitride ceramic material with higher compactness and good thermal conductivity.
With the development of science and technology, the performance requirements on the used materials are higher and higher, and in certain specific fields, aluminum nitride ceramic materials are required to have high thermal conductivity (the thermal conductivity is more than or equal to 200W/(m.K)), and meanwhile, the aluminum nitride ceramic materials with high thermal conductivity and high fracture toughness are required to be developed so as to meet the use requirements of the specific fields.
Disclosure of Invention
The invention aims to provide a low-temperature sintering process of an aluminum nitride ceramic material, which aims to solve the problems in the background technology.
The aim of the invention can be achieved by the following technical scheme:
a low-temperature sintering process of an aluminum nitride ceramic material comprises the following steps:
s1, mixing aluminum nitride powder, nano diamond and a sintering aid to obtain mixed powder;
s2, adding the mixed powder, absolute ethyl alcohol and a ball milling medium into a ball mill according to a mass ratio of 1:1:5-6, and drying, grinding and sieving after ball milling and dispersing uniformly to obtain sintered powder;
s3, adding the sintered powder into a hot-pressing metal mold for compaction to obtain a blank;
and S4, transferring the blank into a graphite mold, and carrying out low-temperature hot-pressing sintering for 2-3 hours under the conditions of the temperature of 1600-1650 ℃ and the pressure of 25-30MPa and nitrogen protection to obtain the aluminum nitride ceramic material.
Further, the average grain diameter of the nano diamond is 5-10nm; the nano diamond is 3-4wt% of aluminum nitride powder. After adding a proper amount of nano diamond into the aluminum nitride powder for sintering, the heat conductivity of the aluminum nitride ceramic material can be improved; on one hand, the nano diamond and the aluminum nitride are both block granular three-dimensional structural materials, belong to hexagonal systems and have similar crystal structures, so that the nano diamond has good compatibility, does not damage crystal grain morphology, has good thermal conductivity, and can improve the thermal conductivity of the aluminum nitride ceramic material; on the other hand, the nano diamond can release amorphous carbon with strong oxygen-expelling effect during sintering, and the amorphous carbon can effectively expel oxygen atoms in aluminum nitride crystal lattice by synergistic action with a multi-element sintering aid, and can reduce deposited yttrium aluminate crystal boundary phase, weaken defect effect of oxygen element and further improve thermal conductivity of aluminum nitride ceramic material.
Further, the nano-diamond is subjected to surface modification treatment before mixing, wherein the nano-diamond is added into a mixed acid solution, magnetically stirred for 1h at 100 ℃, washed to be neutral, and calcined for 1h in a muffle furnace at 400-430 ℃; the nano diamond after acidification and calcination treatment has better dispersibility, so that the nano diamond is uniformly dispersed in aluminum nitride powder during ball milling and mixing, and the negative influence on the mechanical property of the aluminum nitride ceramic material caused by nano diamond agglomeration is avoided.
Further, the usage ratio of the diamond to the mixed acid solution is 1g:50mL, the mixed acid solution is prepared by mixing concentrated nitric acid and concentrated sulfuric acid according to a volume ratio of 1:3.
Further, the sintering aid is Y 2 O 3 CaO and L i 2 O is mixed according to the mass ratio of 3-5:1:2; adding Y 2 O 3 、CaO、L i 2 The multi-element sintering aid composed of O can reduce the sintering temperature and the oxygen content in aluminum nitride crystal lattice.
Further, the sintering aid is used in an amount of 3 to 5wt% of the aluminum nitride powder.
Further, the rotation speed of the ball milling is 300-350r/min, and the ball milling time is 12h.
Further, the drying temperature is 80-100 ℃, the drying time is 6-8 hours, and the mesh number of the screen is 100-200 meshes.
Further, the temperature of the hot-pressing metal mold is 200 ℃, the pressure is 10MPa, and the hot-pressing time is 3 hours.
The invention has the beneficial effects that:
the invention uses the nano diamond and the multi-element sintering auxiliary agent in a matching way, can reduce the sintering temperature, and can obtain the volume density not lower than 3.27g/cm after sintering for 2-3 hours at the temperature of 1600-1650 DEG C 3 The thermal conductivity is not lower than 208W/(m.K), and the fracture toughness is not lower than 3.22 MPa.m 1/2 Aluminum nitride ceramic material of (2);
l i during the sintering of the aluminum nitride powder 2 O and Al 2 O 3 The reaction preferentially generates a liquid phase at 1100 ℃, the wettability of the liquid phase and aluminum nitride crystal grains is improved, and CaO and Y are obviously reduced 2 O 3 And Al 2 O 3 Promoting Y 2 O 3 CaO and Al 2 O 3 Y formed by combination 4 Al 2 O 9 And Ca 3 Al 2 O 6 Aluminate liquid phase, oxygen atoms are bound in the crystal boundary liquid phase, and amorphous carbon generated by nano diamond can be combined with Al 2 O 3 Oxygen is consumed by carbothermic reaction, the thermal conductivity of the aluminum nitride ceramic material is improved, and the redundant amorphous carbon and Y are simultaneously generated 4 Al 2 O 9 The reaction generates aluminum nitride to promote the growth of aluminum nitride crystal, balances the microscopic stress in the material and obviously improves the fracture toughness.
Detailed Description
The technical solutions of the embodiments of the present invention will be clearly and completely described below in conjunction with the embodiments of the present invention, and it is apparent that the described embodiments are only some embodiments of the present invention, not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
Example 1
The embodiment provides a nano diamond, which comprises the following processing steps:
the dosage ratio is 1g:50mL, adding the nano diamond with the particle size of 5nm into a mixed acid solution consisting of concentrated nitric acid and concentrated sulfuric acid according to the volume ratio of 1:3, magnetically stirring and acidizing at 100 ℃ for 1h, washing to be neutral, and calcining at 400 ℃ in a muffle furnace for 1h.
Example 2
The embodiment provides a nano diamond, which comprises the following processing steps:
the dosage ratio is 1g:50mL, adding the nano diamond with the particle size of 8nm into a mixed acid solution consisting of concentrated nitric acid and concentrated sulfuric acid according to the volume ratio of 1:3, magnetically stirring and acidizing at 100 ℃ for 1h, washing to be neutral, and calcining in a muffle furnace at 420 ℃ for 1h.
Example 3
The embodiment provides a nano diamond, which comprises the following processing steps:
the dosage ratio is 1g:50mL, adding the nano diamond with the particle size of 10nm into a mixed acid solution consisting of concentrated nitric acid and concentrated sulfuric acid according to the volume ratio of 1:3, magnetically stirring and acidizing at 100 ℃ for 1h, washing to be neutral, and calcining at 430 ℃ in a muffle furnace for 1h.
Example 4
The embodiment provides a low-temperature sintering process of an aluminum nitride ceramic material, which comprises the following steps of:
step S1, mixing 100g of aluminum nitride powder, 3g of nano diamond obtained in the embodiment 1 and 3g of sintering aid to obtain mixed powder; wherein the sintering aid is Y 2 O 3 CaO and L i 2 O is mixed according to the mass ratio of 3:1:2;
s2, adding the mixed powder, absolute ethyl alcohol and a ball milling medium into a planetary ball mill according to a mass ratio of 1:1:5, uniformly dispersing the mixed powder in the ball mill for 12 hours under the condition of a rotating speed of 300 r/min, drying the mixed powder in a vacuum drying box at 80 ℃ for 8 hours, mechanically grinding the mixed powder, and sieving the mixed powder with a 100-mesh sieve to obtain sintered powder;
s3, adding the sintered powder into a hot-pressing metal mold, and hot-pressing for 3 hours at the temperature of 200 ℃ and the pressure of 10MPa to obtain a blank;
and S4, transferring the blank into a graphite die, and carrying out low-temperature hot-pressing sintering for 3 hours under the conditions of the temperature of 1600 ℃ and the pressure of 25MPa and nitrogen protection to obtain the aluminum nitride ceramic material.
Example 5
The embodiment provides a low-temperature sintering process of an aluminum nitride ceramic material, which comprises the following steps of:
step S1, mixing 100g of aluminum nitride powder, 3g of nano diamond obtained in the embodiment 2 and 4g of sintering aid to obtain mixed powder; wherein the sintering aid is Y 2 O 3 CaO and L i 2 O is mixed according to the mass ratio of 4:1:2;
s2, adding the mixed powder, absolute ethyl alcohol and a ball milling medium into a planetary ball mill according to a mass ratio of 1:1:5, uniformly dispersing the mixed powder in the ball mill for 12 hours under the condition of a rotating speed of 320 r/min, drying the mixed powder in a vacuum drying box at a temperature of 90 ℃ for 7 hours, mechanically grinding the mixed powder, and sieving the mixed powder with a 200-mesh sieve to obtain sintered powder;
s3, adding the sintered powder into a hot-pressing metal mold, and hot-pressing for 3 hours at the temperature of 200 ℃ and the pressure of 10MPa to obtain a blank;
and S4, transferring the blank into a graphite die, and carrying out low-temperature hot-pressing sintering for 3 hours under the conditions of 1630 ℃ and 28MPa of pressure and nitrogen protection to obtain the aluminum nitride ceramic material.
Example 6
The embodiment provides a low-temperature sintering process of an aluminum nitride ceramic material, which comprises the following steps of:
step S1, mixing 100g of aluminum nitride powder, 4g of nano diamond obtained in the embodiment 3 and 5g of sintering aid to obtain mixed powder; wherein the sintering aid is Y 2 O 3 CaO and L i 2 O is mixed according to the mass ratio of 5:1:2;
s2, adding the mixed powder, absolute ethyl alcohol and a ball milling medium into a planetary ball mill according to a mass ratio of 1:1:6, uniformly dispersing the mixed powder in the ball mill for 12 hours under the condition that the rotating speed is 350r/min, drying the mixed powder in a vacuum drying box at 100 ℃ for 6 hours, mechanically grinding the mixed powder, the absolute ethyl alcohol and the ball milling medium, and sieving the mixed powder with a 200-mesh sieve to obtain sintered powder;
s3, adding the sintered powder into a hot-pressing metal mold, and hot-pressing for 3 hours at the temperature of 200 ℃ and the pressure of 10MPa to obtain a blank;
and S4, transferring the blank into a graphite mold, and carrying out low-temperature hot-pressing sintering for 2 hours under the conditions of the temperature of 1650 ℃ and the pressure of 30MPa and nitrogen protection to obtain the aluminum nitride ceramic material.
Comparative example 1
In this comparative example, no nanodiamond was added as compared to example 5, and the remaining process steps and parameters were the same.
Comparative example 2
This comparative example uses only a single Li compared to example 5 2 O is used as a sintering aid, and the rest process steps and parameters are the same.
Comparative example 3
This comparative example uses Y as compared to example 5 2 O 3 And CaO is used as a sintering aid according to the mass ratio of 4:1, and the rest process steps and parameters are the same.
The bulk density, thermal conductivity and fracture toughness were tested for examples 4-6 and comparative examples 1-3 and the results are shown in table 1:
TABLE 1
| Project | Example 4 | Example 5 | Example 6 | Comparative example 1 | Comparative example 2 | Comparative example 3 |
| Bulk Density (g/cm) 3 ) | 3.27 | 3.28 | 3.28 | 3.27 | 3.23 | 3.27 |
| Thermal conductivity (W/(m.K)) | 208 | 218 | 213 | 135 | 176 | 184 |
| Fracture toughness (MPa.m) 1/2 ) | 3.22 | 3.24 | 3.22 | 2.78 | 2.89 | 3.02 |
As can be seen from the data in table 1, the aluminum nitride ceramic materials prepared in examples 4-6 have better compactness, thermal conductivity and fracture toughness; as can be seen from the comparison of the data of comparative examples 1-3 and example 5, the synergistic effect of the nanodiamond and the multi-element sintering aid can significantly improve the thermal conductivity and fracture toughness of the aluminum nitride ceramic material.
It is noted that relational terms such as first and second, and the like are used solely to distinguish one entity or action from another entity or action without necessarily requiring or implying any actual such relationship or order between such entities or actions. Moreover, the terms "comprises," "comprising," or any other variation thereof, are intended to cover a non-exclusive inclusion, such that a process, method, article, or apparatus that comprises a list of elements does not include only those elements but may include other elements not expressly listed or inherent to such process, method, article, or apparatus.
Although embodiments of the present invention have been shown and described, it will be understood by those skilled in the art that various changes, modifications, substitutions and alterations can be made therein without departing from the principles and spirit of the invention, the scope of which is defined in the appended claims and their equivalents.
Claims (9)
1. The low-temperature sintering process of the aluminum nitride ceramic material is characterized by comprising the following steps of:
s1, mixing aluminum nitride powder, nano diamond and a sintering aid to obtain mixed powder;
s2, adding the mixed powder, absolute ethyl alcohol and a ball milling medium into a ball mill according to a mass ratio of 1:1:5-6, and drying, grinding and sieving after ball milling and dispersing uniformly to obtain sintered powder;
s3, adding the sintered powder into a hot-pressing metal mold for compaction to obtain a blank;
and S4, transferring the blank into a graphite mold, and carrying out low-temperature hot-pressing sintering for 2-3 hours under the conditions of the temperature of 1600-1650 ℃ and the pressure of 25-30MPa and nitrogen protection to obtain the aluminum nitride ceramic material.
2. The low temperature sintering process of aluminum nitride ceramic material according to claim 1, wherein the average grain size of the nanodiamond is 5-10nm; the nano diamond is 3-4wt% of aluminum nitride powder.
3. The low temperature sintering process of aluminum nitride ceramic material according to claim 1, wherein the surface modification treatment of the nanodiamond is performed before the mixing, comprising adding the nanodiamond into a mixed acid solution, magnetically stirring for 1h at 100 ℃, washing to neutrality, and calcining for 1h in a muffle furnace at 400-430 ℃.
4. A low temperature sintering process for aluminum nitride ceramic material according to claim 3, wherein the ratio of diamond to mixed acid solution is 1g:50mL, the mixed acid solution is prepared by mixing concentrated nitric acid and concentrated sulfuric acid according to a volume ratio of 1:3.
5. The low temperature sintering process of aluminum nitride ceramic material according to claim 1, wherein the sintering aid is Y 2 O 3 CaO and Li 2 O is mixed according to the mass ratio of 3-5:1:2.
6. The low temperature sintering process of aluminum nitride ceramic material according to claim 5, wherein the sintering aid is used in an amount of 3-5wt% of aluminum nitride powder.
7. The low-temperature sintering process of an aluminum nitride ceramic material according to claim 1, wherein the rotation speed of the ball milling is 300-350r/min, and the ball milling time is 12h.
8. The low temperature sintering process of aluminum nitride ceramic material according to claim 1, wherein the drying temperature is 80-100 ℃, the drying time is 6-8h, and the mesh number is 100-200 mesh.
9. The low temperature sintering process of aluminum nitride ceramic material according to claim 1, wherein the hot pressing metal mold has a temperature of 200 ℃, a pressure of 10MPa, and a hot pressing time of 3 hours.
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