CN102659414B - Easy-sintering AlN polytype-Sialon complex phase material and preparation method thereof - Google Patents
Easy-sintering AlN polytype-Sialon complex phase material and preparation method thereof Download PDFInfo
- Publication number
- CN102659414B CN102659414B CN201210132030.9A CN201210132030A CN102659414B CN 102659414 B CN102659414 B CN 102659414B CN 201210132030 A CN201210132030 A CN 201210132030A CN 102659414 B CN102659414 B CN 102659414B
- Authority
- CN
- China
- Prior art keywords
- sialon
- polytype
- accounts
- sintering
- rare earth
- 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
Links
Images
Landscapes
- Ceramic Products (AREA)
Abstract
The invention relates to an easy-sintering AlN polytype-Sialon complex phase material and a preparation method thereof, which belong to the technical fields of ceramic materials and sintering. According to the method, the AlN polytype-Sialon complex phase material in which an AlN polytype, beta-Sialon, i.e., Si6-zAlzOzN8-z, and U phase Sialon, i.e., Ln3Si3-xAl3+xO12+xN2-x are taken as major phases is prepared from rare earth oxides Ln2O3, Si3N4, AlN, Al2O3 and the like serving as raw materials in an non-oxidizing atmosphere under the atmospheric pressure of 1Pa-10Mpa at the temperature of 1,400-2,000 DEG C for 0.1-12 hours. The rare earth oxide Ln2O3 accounts for 4-15 percent by mass of the total mass of the raw materials; the rare earth element Ln can be La, Ce, Pr, Nd, Sm or Sd; Si3N4 accounts for 27-45 percent by mass of the total mass of the raw materials; AlN accounts for 25-55 percent by mass of the total mass of the raw materials; and Al2O3 accounts for 10-45 percent by mass of the total mass of the raw materials. A related raw material formula has excellent sintering performance; and the prepared Sialon polytype complex phase material has high density, high thermal expansion/contraction performance and excellent mechanical property, and can be applied in the fields of high-temperature-resistant materials, welding and repairing of ceramic components, ceramic assemblies of complex shapes, functional gradient materials and the like.
Description
Technical field
The present invention relates to a kind of easy-sintering A1N polytype-Sialon composite diphase material and preparation method thereof, belong to stupalith and sintering technology field.
Background technology
Silicon nitride (Si
3n
4) be a kind of engineering materials of excellent property, be widely used in each industrial circle.Because its nitrogen content is high, pure silicon nitride ceramics is difficult to sintering, must add sintering aid and could obtain finer and close sintered compact.Last century early seventies, people find the sosoloid of a kind of Si-A1-O-N of containing, i.e. Sialon material when research the affecting of sintering aid.Sialon, as a kind of new engineering material of excellent property, has broad application prospects in fields such as grinding tool and moulding stock, metal cutting tool, Thermal Equipment, smelting iron and steel and chemical machineries.Sialon material comprises the phase that multiple crystalline structure is different, as (with reference to non-patent literatures 1) such as a-Sialon, beta-Sialon, O '-Sialon, X-Sialon, A1N polytype, JEM phase Sialon, S phase Sialon, M phase Sialon, U phase Sialon.Because its structure is different, its mechanical property, physicals and sintering character also there are differences.
In Si-A1-O-N system, there are several Sialon in component between beta-Sialon and A1N, and they have tetrahedron stratiform A1N wurtzite type structure, are referred to as A1N polytype (or being called Sialon polytype).The component of A1N polytype can be used M
mx
m+1represent, wherein M represents atoms metal Si/A1, and X represents non-metallic atom O/N, and m is integer (4≤m≤13).Common several A1N polytypes can be expressed as 8H, 15R, 12H, 21R, 27R and 2H with Ramsdell symbol
δdeng.Because A1N polytype has the pattern of fibrous or en plaque, and most of A1N polytype can coexist mutually with a-Sialon and beta-Sialon, and old friends are generally introduced in above-mentioned materials matrix and rise and strengthen or toughening effect.Different from other Sialon phase performances, although the room temperature folding strength of A1N polytype lower (313～366MPa), it has along with temperature raises, folding strength increases obvious property, can be used as high-temperature structural components etc.Especially at 1000-1300.℃ scope in, their high temperature break resistant intensity surpasses 500MPa (with reference to non-patent literature 2).
Although AIN polytype has superior mechanical behavior under high temperature, its component and A1N approach for ten minutes, and higher nitrogen content makes it be very difficult to sintering.Research in the past all adopts hot-pressing sintering technique, at comparatively high temps (1750～2100.C) under and need to add sintering aid and just can make the densification of A1N polytype.Complicated processing condition and the sintering temperature of superelevation, make A1N polytype material be difficult to realize industrial application.
Patent of the present invention, by composition of raw materials and technological design, obtains a kind of A1N polytype-Sialon composite diphase material with easy-sintering and preparation method thereof.The present invention requires lowly to agglomerating plant, sintering process etc., and can reduce greatly sintering temperature, easily realizes the industrial production of A1N polytype base Sialon composite diphase material.
Non-patent literature 1:S.F.Huang, et a1., Dalton Tran., 40 (2011) 1261-1266.
Non-patent literature 2:H.X.Li, et a1., J. Eur.Ceram.Soc., 15 (1995) 697-701.
Summary of the invention
The object of the invention is to prepare a kind of AlN polytype-Sialon composite diphase material of easy-sintering, make it in easy sintering process appointed condition requirement, and can reduce greatly sintering temperature, easily realize the industrial production of A1N polytype base Sialon composite diphase material.
The preparation method of a kind of easy-sintering A1N polytype-Sialon composite diphase material that the present invention proposes, is characterized in that: with rare earth oxide Ln
2o
3, Si
3n
4, A1N and A1
2o
3for raw material, under non-oxidizing atmosphere, atmosphere pressures 1Pa～10MPa, 1400 ℃～2000 ℃ of temperature, the condition in 0.1 hour～12 hours reaction times, preparing a kind of is Si with A1N polytype, beta-Sialon
6-zal
zo
zn
8-z, and U phase Sialon be Ln
3si
3-xal
3+xo
12+xn
2-xsialon composite diphase material for main phase.
In the preparation method of above-mentioned A1N polytype-Sialon composite diphase material, described rare earth oxide Ln
2o
3the mass ratio that accounts for total batching is 4%～15%, Si
3n
4the mass ratio that accounts for total batching is that the mass ratio that 27%～45%, A1N accounts for total batching is 25%～55%, A1
2o
3the mass ratio that accounts for total batching is 10%～45%, and the weight percent sum of above each feed composition is 100%.
Described preparation method, is characterized in that: described rare earth oxide Ln
2o
3in, rare earth element Ln is selected from La, Ce, Pr, Nd, Sm and Gd.
Described preparation method, is characterized in that: non-oxidizing atmosphere can be selected nitrogen atmosphere, also can select inert gas atmosphere, also can select the mixed-gas atmosphere of rare gas element and nitrogen.
Described preparation method, is characterized in that: atmosphere pressures is 1Pa～10MPa.
A1N polytype-Sialon composite diphase material, is characterized in that: with A1N polytype, beta-Sialon, be Si
6-zal
zo
zn
8-z, and U phase Sialon be Ln
3si
3-xal
3+xo
12+xn
2-xfor main phase.
Described A1N polytype-Sialon composite diphase material, is characterized in that: A1N polytype can be 8H, 15R, 12H, 21R, 27R and 2H
δ, its chemical constitution is respectively SiAl
3o
2n
3, SiAl
4o
2n
4, SiAl
5o
2n
5, SiAl
6o
2n
6, SiAl
8o
2n
8and SiAl
10o
2n
10.
Described A1N polytype-Sialon composite diphase material, is characterized in that: A1N polytype has twin structure.
Described A1N polytype-Sialon composite diphase material, is characterized in that: U phase Sialon is filled in around A1N polytype phase and beta-Sialon phase crystal grain.
Accompanying drawing explanation
Fig. 1 means the electron scanning micrograph of Nd doping A1N polytype-Sialon composite diphase material of the present invention (embodiment 1);
Fig. 2 means the electron scanning micrograph of Pr doping A1N polytype-Sialon composite diphase material of the present invention (embodiment 2).
Embodiment
First the present invention first prepares burden described raw material in described ratio, then pass through mechanical ball milling, make each raw material be mixed evenly rear taking-up and be dried in baking oven, again dried powder is carried out to mechanical pressing, be placed in plumbago crucible and put into high-temperature atmosphere furnace, by described temperature, soaking time and reaction atmosphere condition, reacting; After completing the predetermined reaction times, cool to room temperature, deenergization, takes out sample.
Below by specific embodiment, illustrate in greater detail the present invention, but these embodiment just easily understand the present invention for helping, the present invention is not limited to these embodiment.
Embodiment 1
Select Nd
2o
3, Si
3n
4, A1N and A1
2o
3for raw material, Nd
2o
3the add-on mass percent that accounts for total batching be 9%, Si
3n
4add-on to account for mass percent that add-on that the mass percent of total batching is 35%, A1N accounts for total batching be 37% and A1
2o
3the mass percent that adds total amount to account for total batching be 19%, forming pressure is 200MPa, in nitrogen atmosphere, atmosphere pressures is that 0.9MPa, temperature are 1650 ℃, under the condition that is incubated 3 hours, prepare Nd doping A1N polytype-Sialon composite diphase material, its volume density is 3.40g.cm
-3, apparent porosity is 0.7%, room temperature three-point bending resistance intensity is 335MPa.
Embodiment 2
Select Pr
2o
3, Si
3n
4, A1N and A1
2o
3for raw material, Pr
2o
3the add-on mass percent that accounts for total batching be 11%, Si
3n
4add-on to account for the mass percent that add-on that the mass percent of total batching is 34%, A1N accounts for total batching be 38%, A1
2o
3the mass percent that adds total amount to account for total batching be 17%, forming pressure is 30MPa, in argon gas atmosphere, atmosphere pressures is that 0.12MPa, temperature are 16000, under the condition that is incubated 6 hours, prepare Pr doping A1N polytype-Sialon composite diphase material, its volume density is 3.35g.cm
-3, apparent porosity is 0.8%, room temperature three-point bending resistance intensity is 306MPa.
Claims (6)
1. a preparation method for easy-sintering A1N polytype-Sialon composite diphase material, is characterized in that: with rare earth oxide Ln
2o
3, Si
3n
4, AIN and A1
2o
3for raw material, under non-oxidizing atmosphere, atmosphere pressures 1Pa～10MPa, 1400 ℃～2000 ℃ of temperature, the condition in 0.1 hour～12 hours reaction times, preparing a kind of is Si with A1N polytype, beta-Sialon
6-zal
zo
zn
8-z, and U phase Sialon be Ln
3si
3-xal
3+xo
12+xn
2-xfor the Sialon composite diphase material of main phase, described rare earth oxide Ln
2o
3the mass ratio that accounts for total batching is 4%～15%, Si
3n
4the mass ratio that accounts for total batching is that the mass ratio that 27%～45%, A1N accounts for total batching is 25%～55%, A1
2o
3the mass ratio that accounts for total batching is 10%～45%, and the weight percent sum of above each feed composition is 100%, described rare earth oxide Ln
2o
3in, rare earth element Ln is selected from La, Ce, Pr, Nd, Sm and Gd.
2. preparation method according to claim 1, is characterized in that: non-oxidizing atmosphere is selected nitrogen atmosphere, or selects inert gas atmosphere, or to select the mixed-gas atmosphere of rare gas element and nitrogen, atmosphere pressures be 1Pa～10MPa.
3. easy-sintering A1N polytype-Sialon composite diphase material that according to claim 1 prepared by preparation method, is characterized in that: with A1N polytype, beta-Sialon, be Si
6-za1
zo
zn
8-z, and U phase Sialon be Ln
3si
3-xAl
3+xo
12+xn
2-xfor main phase.
4. A1N polytype-Sialon composite diphase material according to claim 3, is characterized in that: A1N polytype can be 8H, 15R, 12H, 21R, 27R and 2H
δ, its chemical constitution is respectively SiAl
3o
2n
3, SiAl
4o
2n
4, SiAl
5o
2n
5, SiAl
6o
2n
6, SiAl
8o
2n
8and SiAl
10o
2n
10.
5. A1N polytype-Sialon composite diphase material according to claim 3, is characterized in that: A1N polytype has twin structure.
6. A1N polytype-Sialon composite diphase material according to claim 3, is characterized in that: U phase Sialon is filled in around A1N polytype phase and beta-Sialon phase crystal grain.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201210132030.9A CN102659414B (en) | 2012-02-24 | 2012-05-02 | Easy-sintering AlN polytype-Sialon complex phase material and preparation method thereof |
Applications Claiming Priority (3)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201210046127 | 2012-02-24 | ||
| CN201210046127.8 | 2012-02-24 | ||
| CN201210132030.9A CN102659414B (en) | 2012-02-24 | 2012-05-02 | Easy-sintering AlN polytype-Sialon complex phase material and preparation method thereof |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN102659414A CN102659414A (en) | 2012-09-12 |
| CN102659414B true CN102659414B (en) | 2014-01-15 |
Family
ID=46769029
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN201210132030.9A Active CN102659414B (en) | 2012-02-24 | 2012-05-02 | Easy-sintering AlN polytype-Sialon complex phase material and preparation method thereof |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN102659414B (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP3218323A4 (en) * | 2014-11-13 | 2018-07-11 | Taegutec Ltd. | Ceramic material and cutting tools made thereof |
Families Citing this family (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US9695087B2 (en) | 2013-12-27 | 2017-07-04 | Ngk Spark Plug Co., Ltd. | Sialon sintered body and cutting insert |
| JP6697363B2 (en) * | 2015-10-30 | 2020-05-20 | 日本碍子株式会社 | Semiconductor manufacturing equipment member, manufacturing method thereof, and heater with shaft |
Family Cites Families (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1304331C (en) * | 2005-03-31 | 2007-03-14 | 北京科技大学 | Compound phose material of beta cellulose and alpha cellulose and its preparation technology |
| CN101560100A (en) * | 2009-05-27 | 2009-10-21 | 东北大学 | Method for preparing O'-Sialon/AIN composite powder |
| CN101748488A (en) * | 2009-12-21 | 2010-06-23 | 中国地质大学（北京） | Novel rare-earth Ln-Sialon mono-crystal and preparation method thereof |
-
2012
- 2012-05-02 CN CN201210132030.9A patent/CN102659414B/en active Active
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP3218323A4 (en) * | 2014-11-13 | 2018-07-11 | Taegutec Ltd. | Ceramic material and cutting tools made thereof |
Also Published As
| Publication number | Publication date |
|---|---|
| CN102659414A (en) | 2012-09-12 |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| Ceja-Cárdenas et al. | Spark plasma sintering of α-Si3N4 ceramics with Al2O3 and Y2O3 as additives and its morphology transformation | |
| CN102115332B (en) | High-strength beta-SiAlON ceramic and pressureless sintering preparation method thereof | |
| CN108439995B (en) | Complex phase ceramic and preparation method thereof | |
| CN112851365B (en) | Preparation method of silicon nitride-based complex phase conductive ceramic | |
| Zawrah et al. | Liquid-phase sintering of SiC in presence of CaO | |
| CN110590377A (en) | High beta-phase compact silicon nitride ceramic and low-temperature preparation method | |
| CN102659414B (en) | Easy-sintering AlN polytype-Sialon complex phase material and preparation method thereof | |
| JP5046221B2 (en) | Manufacturing method of highly reliable silicon nitride ceramics with high reliability | |
| CN106747474B (en) | Preparation method of high-thermal-conductivity silicon nitride ceramic | |
| Chen | Effects of gadolinia and alumina addition on the densification and toughening of silicon carbide | |
| Lee et al. | Effect of raw-Si particle size on the properties of sintered reaction-bonded silicon nitride | |
| Hongsheng et al. | Fabrication of β-Si3N4 with high thermal conductivity under ultra-high pressure | |
| CN110627507A (en) | Low-temperature silicon carbide ceramic and preparation method and application thereof | |
| Ma et al. | Processing and microstructure characterization of liquid-phase-sintered, α-SiC matrix composites | |
| CN107473730B (en) | Method for preparing fine-grain and high-strength magnesia-alumina spinel transparent ceramic | |
| CN103011872A (en) | Preparation method of silicon nitride toughening ceramic | |
| Santos et al. | α-SiAlON–SiC composites obtained by gas-pressure sintering and hot-pressing | |
| CN109400176A (en) | A kind of high-performance silicon nitride ceramics and its preparation method and application | |
| Bandyopadhyay | The in situ formation of Sialon composite phases | |
| CN101748488A (en) | Novel rare-earth Ln-Sialon mono-crystal and preparation method thereof | |
| CN103848639A (en) | Silicon nitride toughened ceramic | |
| CN107619289B (en) | Preparation method of whisker self-toughening alpha-SiAlON ceramic material | |
| CN101955357A (en) | Processable complex-phase ceramic material and preparation method thereof as well as secondary hardening heat treatment method | |
| CN101956115B (en) | Processable complex phase ceramic material and preparation method and secondary hardening heat treatment method thereof | |
| JP3007732B2 (en) | Silicon nitride-mixed oxide sintered body and method for producing the same |
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 |