CN1301935C - Process for preparing AIN ceramic material - Google Patents
Process for preparing AIN ceramic material Download PDFInfo
- Publication number
- CN1301935C CN1301935C CNB2005100213795A CN200510021379A CN1301935C CN 1301935 C CN1301935 C CN 1301935C CN B2005100213795 A CNB2005100213795 A CN B2005100213795A CN 200510021379 A CN200510021379 A CN 200510021379A CN 1301935 C CN1301935 C CN 1301935C
- Authority
- CN
- China
- Prior art keywords
- aln
- sintering
- sintering aid
- mould
- pressure
- 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.)
- Expired - Fee Related
Links
Landscapes
- Ceramic Products (AREA)
Abstract
The present invention discloses a making method of high-performance AlN ceramics, which comprises: 1. AlN powder is prepressed into sheets by steel moulds at room temperature at the pressure of 30MPa to 60MPa; 2. the prepressed AlN sheet samples are put into a cool isostatic pressing machine for cool isotactic pressing at the pressure of 200MPa to 250MPa; 3. after the cool isotactic pressing, the samples are put into a molybdenum cup, the molybdenum cup is put into a dolomite insulation cup, the insulation cup is put into a graphite heating medium which is then put into a dolomite mould, and the dolomite is used as the pressure transmitting medium; 4. the dolomite mould with the AlN samples is put into a belt-type press to be pressurized to 4GPa to 8GPa and then heated, the temperature is raised to 1500 DEG C to 1750 DEG C and preserved for certain time in the conditions of high pressure and high temperature, then the mould is naturally cooled, and the making of the AlN ceramics is completed. The method provided by the present invention has the advantages of simple process, practicality, easy operation, low sintering temperature, short sintering time and production periodicity, low cost and excellent performance of the obtained AlN ceramic materials.
Description
Technical field
The invention belongs to field of ceramic material preparation, be specifically related to a kind of preparation method of AlN stupalith.
The present invention is mainly used in AlN, SiC, the Si of preparation sintering difficulty
3N
4, ZrO
2Structural ceramics and functional materials Deng a big class excellent performance.
By enforcement of the present invention, can obtain the AlN stupalith of densification, no obvious crystal boundary, thereby salient featuress such as its thermal conductivity, volume specific resistance, disruptive strength are increased substantially, specific inductivity reduces, and satisfies the requirement of industrial technology field to high thermal conductivity, high performance AlN substrate material, AlN heat sink material and AlN high-temperature structural material.
Background technology
The AlN pottery has the not high and advantages such as dielectric loss is lower, physical strength is high, excellent electric insulation, the thermal expansivity, stable chemical performance, the resistance to elevated temperatures that are complementary with silicon are good, high-temperature mechanics intensity big, good toughness and nontoxicity of high heat conductance, specific inductivity, its thermal conductivity theoretical value is 320W/m.k, is about Al
2O
310 times, thermal expansivity is 4.5 * 10
-6℃
-1Approaching with Si, material non-toxic, be convenient to processing and manufacturing, be the desirable heat sink material and the packaged material of large-scale integrated circuit, semiconductor module circuit and high power device, being subjected to the favor of countries in the world, being regarded as the rising superior isolation heat dispersion substrate material of a new generation, also is the high-temperature structural material of excellent performance simultaneously.
In recent years, people are by the big quantity research to the AlN pottery, be fully recognized that the gordian technique of obtaining high thermal conductance, high-performance AlN pottery is the control of feed oxygen content, eliminating and microstructure (size of grain-size and the distribution of sintered compact oxygen impurities, the crystal boundary state, void content and stomata states, the content of impurity and distribution etc.) control.Aspect the eliminating of the control of AlN feed oxygen content, sintered compact oxygen impurities, multiple powder preparing, thermal treatment process and sintering aid have been developed, make oxygen level and other impurity of AlN pottery obtain effective control, but, the sintering of AlN pottery undesirable (microstructure is not well controlled), influenced the performance of AlN pottery to a great extent, the sintering technology that exploitation AlN pottery is new is significant to the performance that improves the AlN pottery.
Chinese patent literature notification number CN1099739 discloses the patented technology that a kind of name is called " reaction sintering is used to prepare aluminium nitride and composite ceramics thereof ", be characterized in mixed powder that method that reaction sintering is used to prepare aluminium nitride and composite ceramics thereof is to contain aluminium powder by ball milling, vacuum drying, sieve, cold isostatic compaction, preprocessing, technological processs such as nitrogenizing reaction sintering obtain fine and close finished product at last.Prepare aluminium nitride and composite ceramics thereof with the reaction sintering technology, it is relatively low to have a preparation temperature, and the raw material of employing cheaply is easy to get, and newly-generated aluminum nitride grain is tiny, and sintered compact does not almost shrink, preparation cost is lower etc.Its weak point is the sintering difficulty, and the sintering period is long, and production cost is higher, and microstructure is undesirable, crystal grain is big, crystal boundary obviously, easily electrical breakdown, poor surface smoothness.
Mainly there is following problem in the production method of AlN pottery of the prior art:
(1) AlN and SiC, BN, Si
3N
4, B
4Non-oxidized substances such as C are the same, sintering difficulty under the normal pressure atmosphere protection.At present, the AlN pottery is at N
2Sintering temperature in the atmosphere, more than 1800 ℃, soaking time reaches 4 hours, sintering period is long, production cost is higher, but its microstructure is undesirable, have defectives such as crystal grain is big, pore is big, void content is higher, crystal boundary is obvious, important performance index such as the surface smoothness after thermal conductivity, electric breakdown strength, the polishing are undesirable.
(2) present, the AlN Production of Ceramics need be passed through the anti-aquation pre-treatment of raw material, N
2Fine grinding, flow casting molding, thermal treatment under the protection is come unstuck, high temperature N
2Technologies such as sintering under the protection exist production link many, complex process, and it is big to grasp the gordian technique difficulty, and the product performance fluctuation is bigger, shortcomings such as production cost height.
Summary of the invention
The preparation method who the purpose of this invention is to provide a kind of AlN pottery of high surface finish.
Purpose of the present invention is achieved by the gordian technique and the production cost control of AlN Production of Ceramics, improve at aspects such as the design of the pre-treatment of sintering aid, sintering mold, ultra-high voltage hot pressed sinterings, the content of microstructure, oxygen level and other impurity of control AlN pottery, the excellent performance of the AlN stupalith of acquisition, surface smoothness height.
The present invention utilizes belt type press to be agglomerating plant, realizes 4GPa ~ 8GPa ultra-high voltage, low temperature, the Fast Sintering of stupalith, obtained performance excellence, the AlN pottery that production cost is low.
The preparation method of a kind of AlN pottery of the present invention mainly comprises the steps:
A. the pre-treatment of sintering aid
With sintering aid fine grinding 1～8 hour;
The grinding of b.AlN raw material and sintering aid
The AlN material powder adds the common grinding of pretreated sintering aid 1～8 hour.
C. vacuum drying oven
With the powder of AlN raw material after grinding and sintering aid in vacuum drying oven dry 1～5 hour.
D. sintering mold selects for use
Under the pressure of 20MPa～50MPa, with punching block will prepare burden, the pre-tablet forming of AlN powder after the fine grinding;
E. cold isostatic compaction
Under the pressure of 200MPa～250MPa, with the base substrate of a plurality of pre-moldings, cold isostatic compaction is made the flake shaped base substrate of AlN;
F.AlN powder pre-molding
The AlN base substrate of forming is adorned as putting into the molybdenum cup, and the molybdenum cup is put into the core insulator of rhombspar, and core insulator is put into the heating graphite medium, and then in the rhombspar mould of packing into; The rhombspar mould that the AlN sample is housed is packed in the belt type press;
G. adopting belt type press is agglomerating plant, carry out AlN pottery low temperature, fast, the sintering of oxygen-free atmosphere control
Be pressurized to 4Gpa～8Gpa earlier, begin to heat to 1500 ℃～1750 ℃ then, be incubated 60～120 minutes, naturally cooling.
Sintering aid adopts Y
2O
3, Sm
2o
3, Dy
2O
3, Nd
2O
3Or Y
2O
3And Dy
2O
3In a kind of.
In the preparation process of AlN pottery of the present invention
(1) pre-treatment of sintering aid
With Y
2O
3, Sm
2o
3, Dy
2O
3, Nd
2O
3Or Y
2O
3And Dy
2O
3Deng sintering aid fine grinding before batching, 1～8 hour, reducing its granularity, guarantee that sintering aid and AlN powder mix, bring into play to greatest extent sintering aid deoxidation, help the agglomerating effect.
(2) sintering mold selects for use
To select rhombspar for use be the dielectric material and wear the piezodielectric material.
Rhombspar does not have reversible phase transformation, chemical reaction under high pressure-temperature, and has the characteristics of high coefficient of thermal expansion, to improving the sintering cavity pressure, guarantees that 4GPa～8GPa ultra-high voltage hot pressed sintering is significant.
(3) AlN powder pre-molding
With punching block will prepare burden, the pre-tablet forming of AlN powder after the fine grinding, the flake shaped base substrate of cold isotactic compaction AlN under the pressure of 200MPa～250MPa, purpose is in order to obtain the fine and close base substrate of AlN uniformly.
(4) adopting belt type press is agglomerating plant, carries out the sintering of AlN pottery low temperature, quick, no atmosphere control
The AlN base substrate of forming is adorned as putting into the molybdenum cup, can be prevented that sample is contaminated in the sintering process, have to guarantee that base substrate is subjected to uniform high pressure effect when sintering; Then the molybdenum cup is put into the core insulator of rhombspar, core insulator is put into the heating graphite medium, in the rhombspar mould of will packing into again, rhombspar is as transmission medium; The rhombspar mould that installs the AlN sample is packed in the belt type press, begin heating after being pressurized to 4GPa～8GPa earlier, be warmed up to 1500 ℃～1750 ℃, under this high pressure, hot conditions, be incubated 60～120 minutes, naturally cooling is finished the preparation of AlN pottery then.The sintering period that comprises heating-up time, temperature fall time, soaking time is 70～130 minutes.
The present invention is agglomerating plant with the belt type press, adopt the ultra-high voltage (hot pressing and sintering technique of 4GPa～8GPa), the AlN stupalith of preparation densification, uniform microstructure, no obvious crystal boundary, its performance and sintering degree are better than the AlN stupalith of ordinary method preparation.
Prepare the AlN method of ceramic material with routine and compare, the present invention has the following advantages:
(1) the present invention adopts the sintering technology of ultra-high voltage, low temperature, quick, no atmosphere control, and performances such as the thermal conductivity of acquisition AlN pottery, volume specific resistance, disruptive strength, surface smoothness increase substantially, and cost is lower;
(2) technology of the present invention is simple, practical, easy handling, and sintering temperature is low, sintering time and with short production cycle, cost is low.Do not need the AlN powder is carried out anti-aquation pre-treatment, do not need to adopt the casting method moulding, saved the thermal treatment degumming technology.
Description of drawings
Fig. 1 is the process flow sheet of AlN pottery of the present invention preparation
Embodiment
The present invention is described in further detail below in conjunction with accompanying drawing.
As can be seen, the preparation process of a kind of AlN pottery of the present invention mainly comprises the steps: from the process flow sheet of Fig. 1 AlN pottery of the present invention preparation
(1) pre-treatment of sintering aid
With Y
2O
3And Dy
2O
3Complex sintering aids ground 3 hours in the mill fast.
(2) grinding of AlN raw material and sintering aid
The AlN material powder adds the pretreated Y of 5wt%
2O
3And Dy
2O
3Complex sintering aids is common to be ground 1 hour.Y wherein
2O
3Addition be 4wt%, Dy
2O
3Add-on be 1wt%.
(3) vacuum drying oven
With the powder of AlN raw material after grinding and sintering aid in vacuum drying oven dry 1 hour.
(4) AlN powder pre-molding
With AlN powder after the vacuum-drying, under 30Mpa pressure, be pre-pressed into the disk shape base substrate of φ 25mm.
(5) cold isostatic compaction
With the mantle mould that the base substrate of a plurality of pre-moldings is put into, cold isostatic compaction under the pressure of 250MPa.
(6) adopting belt type press is agglomerating plant, has realized the sintering that AlN pottery low temperature, quick, no atmosphere are controlled
The AlN base substrate of forming is adorned as putting into the molybdenum cup, in case the pollution in the sintering process; Then the molybdenum cup is put into the core insulator of rhombspar, core insulator is put into the heating graphite medium, in the rhombspar mould of will packing into again, rhombspar is as transmission medium; To install AlN sample rhombspar mould and pack in the belt type press, and begin heating after being pressurized to 5.15GPa earlier, and be warmed up to 1675 ℃, and under this high pressure, hot conditions, be incubated 100 minutes, naturally cooling is finished the preparation of AlN pottery then.The sintering period that comprises heating-up time, temperature fall time, soaking time is about 115 minutes.
(7) polishing, cleaning
Use diamond abrasive, the AlN ceramic surface is carried out fine grinding, polished finish.Soak the AlN pottery that has polished with dilute hydrochloric acid, tap water cleans.
The Specifeca tion speeification of the AlN pottery of preparation sees Table 1.
The Specifeca tion speeification of table 1 AlN pottery
| Performance index | The AlN ceramic substrate |
| Thermal conductivity (w/m.k) | 202 |
| Density (g/cm3) | 3.31 |
| Volume specific resistance (Ω cm, 25 ℃) | 1.3×10 15 |
| Specific inductivity (1MHz, 25 ℃) | 6.0 |
| Dielectric loss factor (1MHz, 25 ℃) | 9.8×10 4 |
| Disruptive strength (KV/mm, 25 ℃) | 31.8 |
| Thermal expansivity (10 -6/℃，25℃～300℃) | 4.25 |
| Breaking tenacity (MPa, 25 ℃) | 400 |
| Microhardness (GPa, 25 ℃) | 8.8 |
| Surface smoothness | 0.1μm |
Claims (2)
1, a kind of preparation method of AlN pottery is characterized in that preparation process mainly may further comprise the steps:
A. the pre-treatment of sintering aid
With sintering aid fine grinding 1～8 hour;
The grinding of b.AlN raw material and sintering aid
The AlN material powder adds the common grinding of pretreated sintering aid 1～8 hour;
C. vacuum drying oven
With the powder of AlN raw material after grinding and sintering aid in vacuum drying oven dry 1～5 hour;
D. sintering mold selects for use
Under the pressure of 20Mpa～50MPa, with punching block will prepare burden, the pre-tablet forming of AlN powder after the fine grinding;
E. cold isostatic compaction
Under the pressure of 200MPa～250MPa, with the base substrate of a plurality of pre-moldings, cold isostatic compaction is made the flake shaped base substrate of AlN;
F.AlN powder pre-molding
The AlN base substrate of forming is adorned as putting into the molybdenum cup, and the molybdenum cup is put into the core insulator of rhombspar, and core insulator is put into the heating graphite medium, and then in the rhombspar mould of packing into; The rhombspar mould that the AlN sample is housed is packed in the belt type press;
G. adopting belt type press is agglomerating plant, carry out AlN pottery low temperature, fast, the sintering of oxygen-free atmosphere control
Be pressurized to 4Gpa～8Gpa earlier, begin to heat to 1500 ℃～1750 ℃ then, be incubated 60～120 minutes, naturally cooling.
2, the preparation method of a kind of AlN pottery according to claim 1 is characterized in that: sintering aid adopts Y
2O
3, Sm
2o
3, Dy
2O
3, Nd
2O
3Or Y
2O
3And Dy
2O
3In a kind of.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNB2005100213795A CN1301935C (en) | 2005-07-29 | 2005-07-29 | Process for preparing AIN ceramic material |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNB2005100213795A CN1301935C (en) | 2005-07-29 | 2005-07-29 | Process for preparing AIN ceramic material |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN1749213A CN1749213A (en) | 2006-03-22 |
| CN1301935C true CN1301935C (en) | 2007-02-28 |
Family
ID=36604893
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CNB2005100213795A Expired - Fee Related CN1301935C (en) | 2005-07-29 | 2005-07-29 | Process for preparing AIN ceramic material |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN1301935C (en) |
Families Citing this family (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101570437B (en) * | 2009-04-30 | 2013-01-09 | 潮州三环（集团）股份有限公司 | Method for continuous low temperature sintering of high thermal coefficient AIN ceramics and product thereof |
| CN101948315A (en) * | 2010-09-21 | 2011-01-19 | 上海理工大学 | Low-temperature sintering method of high-performance aluminium nitride ceramics |
| CN102875156A (en) * | 2012-10-08 | 2013-01-16 | 广东顺祥节能照明科技有限公司 | Preparation method of aluminum nitride ceramic LED lamp thermal-conducting material |
| CN103011830A (en) * | 2012-12-31 | 2013-04-03 | 河南理工大学 | Ultrahigh-pressure low-temperature sintering preparation method of transparent aluminium nitride ceramic |
| GB201307804D0 (en) | 2013-04-30 | 2013-06-12 | Element Six Ltd | Composite material, articles comprising same and method for making same |
| CN107954725B (en) * | 2017-11-29 | 2021-03-30 | 上海宇昂水性新材料科技股份有限公司 | Hydrolysis-resistant aluminum nitride powder and preparation method thereof |
Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0471568B1 (en) * | 1990-08-15 | 1995-08-30 | The Dow Chemical Company | A self-reinforced silicon nitride ceramic body and a method of preparing the same |
| CN1130607A (en) * | 1995-11-17 | 1996-09-11 | 清华大学 | Method for manufacturing high-heat conductivity aluminium nitride ceramics |
| CN1203898A (en) * | 1998-07-08 | 1999-01-06 | 中国科学院上海硅酸盐研究所 | Low temp. sintering of aluminum nitride ceramics |
| EP0695732B1 (en) * | 1994-08-02 | 2000-01-12 | Sumitomo Electric Industries, Ltd. | Metallized ceramic substrate having smooth plating layer and method for producing the same |
-
2005
- 2005-07-29 CN CNB2005100213795A patent/CN1301935C/en not_active Expired - Fee Related
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0471568B1 (en) * | 1990-08-15 | 1995-08-30 | The Dow Chemical Company | A self-reinforced silicon nitride ceramic body and a method of preparing the same |
| EP0695732B1 (en) * | 1994-08-02 | 2000-01-12 | Sumitomo Electric Industries, Ltd. | Metallized ceramic substrate having smooth plating layer and method for producing the same |
| CN1130607A (en) * | 1995-11-17 | 1996-09-11 | 清华大学 | Method for manufacturing high-heat conductivity aluminium nitride ceramics |
| CN1203898A (en) * | 1998-07-08 | 1999-01-06 | 中国科学院上海硅酸盐研究所 | Low temp. sintering of aluminum nitride ceramics |
Also Published As
| Publication number | Publication date |
|---|---|
| CN1749213A (en) | 2006-03-22 |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| CN1301935C (en) | Process for preparing AIN ceramic material | |
| CN101050115A (en) | Ceramics of containing powder body of cubic silicon nitride, and preparation method | |
| CN107188567B (en) | Preparation method of aluminum nitride ceramic with high thermal conductivity | |
| CN102219536B (en) | B4C/SiC whisker/SiC multiphase ceramic matrix composite and preparation method thereof | |
| CN102272074B (en) | Large ceramic component and method of manufacture | |
| CN102161594B (en) | SiC whisker reinforced SiC ceramic matrix composite and preparation method thereof | |
| CN110128146B (en) | Multifunctional boron carbide-based multiphase ceramic and reactive hot-pressing sintering preparation method thereof | |
| CN1600742A (en) | Compact foamy thyrite in high intensity and preparation method | |
| CN101648809B (en) | Boron nitride based composite ceramic wave-transparent material and preparation method thereof | |
| CN101255057B (en) | Silicon nitride porous ceramic composition and preparation method thereof | |
| CN102070341A (en) | Preparation method for microwave solid-state synthesis of self-toughening silicon nitride ceramic | |
| CN105503254A (en) | Barium titanate foamed ceramic and preparing method thereof | |
| CN101734923A (en) | Aluminum nitride porous ceramic and preparation method thereof | |
| CN112939607A (en) | High-thermal-conductivity aluminum nitride ceramic and preparation method thereof | |
| CN108751996A (en) | A kind of the boron carbide ceramics material and its plasma agglomeration preparation process of graphene toughening | |
| CN110436928A (en) | High-performance nano twin boron carbide ceramics block materials and preparation method thereof | |
| CN102786304B (en) | Preparation method for hot-pressed boron carbide ceramic | |
| CN111116202A (en) | Method for sintering boron carbide-titanium boride material through discharge plasma reaction | |
| JP2002187774A5 (en) | ||
| CN103755353B (en) | A kind of fast low temperature preparation method of Y-α-SiAlON crystalline ceramics | |
| CN109732088A (en) | A kind of novel composite ceramic that thermal shock resistance is high and its processing technology | |
| CN112919915A (en) | Method for pressing silicon nitride ceramic special-shaped cutter by SPS pressure sintering powder | |
| CN101885608A (en) | Boron nitride nanotube strengthened silicon nitride ceramic material and preparation method thereof | |
| CN101182211B (en) | Nano silicon carbide ceramic preparation method | |
| CN114349516B (en) | Method for synthesizing high-density SiC ceramic at low temperature |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| C06 | Publication | ||
| PB01 | Publication | ||
| C10 | Entry into substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| C14 | Grant of patent or utility model | ||
| GR01 | Patent grant | ||
| C17 | Cessation of patent right | ||
| CF01 | Termination of patent right due to non-payment of annual fee |
Granted publication date: 20070228 Termination date: 20110729 |