CN100355701C - Prepn process of SiN ceramic with high heat conductivity - Google Patents

Prepn process of SiN ceramic with high heat conductivity Download PDF

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Publication number
CN100355701C
CN100355701C CNB200610024154XA CN200610024154A CN100355701C CN 100355701 C CN100355701 C CN 100355701C CN B200610024154X A CNB200610024154X A CN B200610024154XA CN 200610024154 A CN200610024154 A CN 200610024154A CN 100355701 C CN100355701 C CN 100355701C
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sintering
high heat
heat conductivity
preparation
ceramics
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CN1810720A (en
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彭桂花
江国健
李文兰
张宝林
庄汉锐
徐素英
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Shanghai Institute of Ceramics of CAS
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Shanghai Institute of Ceramics of CAS
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Abstract

The present invention relates to a preparation method for high heat conducting Si3N4 ceramics, which is characterized in that an SPS low-temperature rapid sintering technology and a method for preparing high heat conducting silicon nitride ceramics taking nitride as sintering aids are adopted and belongs to the field of non-oxide ceramics preparation. The high heat conducting Si3N4 ceramics are mixed by alpha-Si3N4 powder and the sintering aids according to the proportion of 100: 10 to 2 and are prepared by the SPS low-temperature rapid sintering technology. During the preparation, raw materials are filled in a graphite mould and are rapidly sintered by SPS under the conditions of 10 to 100MPa, 1500 DEG C to 1700 DEG C, and 3 to 30 minutes of heat preservation time. The silicon nitride ceramics prepared by the present invention has high thermal conductivity and still maintains high strength simultaneously, the heat conductivity can reach 120Wm<-1>K<-1>, and the three point folding strength sigma b reaches more than 750MPa.

Description

A kind of preparation method of SiN ceramic with high heat conductivity
Technical field
The present invention relates to a kind of preparation method of SiN ceramic with high heat conductivity, more precisely be to prepare the method for SiN ceramic with high heat conductivity as the low temperature Fast Sintering of the discharge plasma sintering (SPS) of sintering aid, belong to the non-oxide ceramics preparation field with nitride powder.
Background technology
In recent years, people find Si in the high thermo-conductive ceramic substrate material process of research 3N 4Meet the feature of Slack about high thermal conducting material.Haggerty and Lightfoot are according to Si 3N 4Structure β-Si is proposed 3N 4Theoretical thermal conductivity up to 200～320W/mK, but also have thermal expansivity and very excellent performance such as single crystalline Si is approaching, electrical insulating property is good, nontoxic, be a kind of ideal heat radiation and packaged material.
Si 3N 4Pottery and AlN ceramic phase ratio have irreplaceable advantage, Si 3N 4Ceramics strength reaches more than the 600MPa easily, is more than AlN pottery (about 300MPa) the intensity twice, under the identical situation of heat dissipation capacity, and Si 3N 4Even ceramic substrate do the thinner requirement that still can satisfy intensity; Si 3N 4Oxidation-resistance is stronger than AlN, can water basely handle, thereby can reduce cost greatly.In addition, Si 3N 4Also have a series of unique excellent physics, chemical properties under normal temperature and the high temperature, as high tenacity, low thermal coefficient of expansion, resistance to sudden heating, good insulation performance, wear-resistant and corrosion-resistant etc., and property retention to temperature reaches 1000 ℃ of not obvious declines.
Si 3N 4The thermal conductance of pottery is relevant with the mean free path of phon scattering, and the latter and Si 3N 4Perfection of lattice relevant with crystal boundary, influence Si 3N 4The microtexture defective of heat conductivility can be divided into two big classes, and the first kind is Si 3N 4The crystal grain subsurface defect is as crystal grain defectives such as lattice imperfections such as lattice distortion, room, dislocation, fault, antiphase domain boundary and intracrystalline precipitate, Solid solution, bubble, wherein Si 3N 4Oxygen level is to Si in the pottery 3N 4The thermal conductance influence of pottery is very big; Another kind of is grain boundary defects, comprises that crystal boundary state, crystal boundary second phase, pore and glass equate.Studies show that wherein the oxygen in the lattice is to Si 3N 4The thermal conductivity influence of pottery is very big.
The researchist is studying energetically with oxide compound how to obtain high thermal conductance, high performance Si as sintering aid both at home and abroad 3N 4Pottery.Wherein Ri Ben H.Yokota etc. adopts the Yb of 10mass% 2O 3ZrO with 2mass% 2As sintering aid; under the nitrogen protection of 0.9Mpa; earlier 1900 ℃ of insulations 36 hours; then 1700 ℃ of insulations 100 hours; obtaining thermal conductivity is the silicon nitride ceramics [H.Yokota of 150W/mK; H.Abe, M.Ibukiyama, Effect of lattice defects on the thermal conductivity of β-Si 3N 4, J.Eur.Ceram.Soc., 23 (2003) 1751-1759].How domestic Tsing-Hua University also prepares the SiN ceramic with high heat conductivity material in active research, but its highest thermal conductivity has only 79W/mK[Wei Xu, Xiao-shanNing, He-ping Zhou, Yuan-bo Lin, Study on the thermal conductivity andmicrostructure of silicon nitride used for power electronic substrate, Mater.Sci.Eng.B, 99 (2003) 475-478].
The SPS low temperature Fast Sintering technology that developed recently gets up has characteristics such as temperature rise rate is fast, sintering time is short, sintering structure is even.The researchist is applied to SPS low temperature Fast Sintering technology the sintering of various potteries just energetically both at home and abroad.[Zhijian Shen such as doctor Shen Zhijian of Stockholm Univ Sweden, Zhe Zhao, Hong Peng, Mats Nygren, Formation of tough interlocking microstructuresin silicon nitride ceramics by dynamic ripening, Nature, 417 (2002) 266-269] propose to adopt SPS low temperature Fast Sintering technology, can under lower temperature, obtain the silicon nitride ceramics that crystal grain is fully grown up.
Can the present invention intends creationary proposition with nitride as sintering aid, the silicon nitride ceramics for preparing high thermal conductance by SPS low temperature Fast Sintering method, reduced on the one hand that impurity oxygen is to the influence of final ceramic performance in the oxidesintering auxiliary agent that the conventional silicon nitride pottery adopted, the extremely short soaking time of low on the other hand temperature can reduce expending of the energy and manpower greatly.The silicon nitride ceramics of this invention preparation can reach high thermal, has reached 120W/mK, and has kept mechanical property preferably.Up to the present, do not see the report that is equipped with SiN ceramic with high heat conductivity separately with nitride as sintering aid SPS low temperature Fast Sintering legal system as yet.
Summary of the invention
The object of the present invention is to provide a kind of preparation method of silicon nitride ceramics of high thermal conductance.
Specifically:
(1) with α-Si 3N 4Powder and be starting raw material as the nitride powder of sintering aid, both part by weight are 100: 10～2; α-Si wherein 3N 4α phase content＞the 83wt% of powder, nitride are MgSiN 2, Mg 3N 2And BeSiN 2In any one powder or their mixture, its purity＞98wt%, particle diameter are 0.3～10 μ m.
(2) with after containing the powder uniform mixing of sintering aid in the above-mentioned steps, in the graphite jig of packing into then, SPS low temperature Fast Sintering under 10～100MPa, 1500 ℃～1700 ℃, 3～30 minutes condition of soaking time.Sintering finishes the back sample and cools to room temperature with the furnace; Atmosphere is vacuum or nitrogen protection during the SPS sintering; The direction consistent (promptly parallel) of pulsed current direction and pressurization.
Obviously, the preparation method of SiN ceramic with high heat conductivity provided by the invention compares with the preparation method of existing silicon nitride ceramics, has following advantage:
(1) prepares the compact silicon nitride pottery with less relatively sintering aid;
(2) under lower temperature and low pressure and in the pressure condition under prepare high thermal conductance, high-intensity silicon nitride ceramics;
(3) under short soaking time, prepare the silicon nitride ceramics of high thermal conductance;
(4) prepared silicon nitride ceramics has good calorifics, mechanical property, and wherein thermal conductivity reaches as high as 120W/mK, 3 folding strength σ between 50～120W/mK bReach more than the 750MPa.
Description of drawings
Fig. 1 is a process flow sheet of the present invention
Fig. 2 is the polished surface erosion profile figure of the silicon nitride ceramics of embodiment 1 gained provided by the present invention
Embodiment
Further illustrate characteristics of the present invention below by embodiment, but be not limited to embodiment.
Embodiment 1
To add 3wt% sintering aid MgSiN 2The powder uniform mixing after, in the graphite jig of packing into then, SPS sintering under 60MPa, 1500 ℃, 12 minutes condition of soaking time.Sintering finishes the back sample and cools to room temperature with the furnace.
Silicon nitride ceramics thermal conductivity by above-mentioned prepared can reach 100W/mK, 3 folding strength σ bReach 946MPa, Vickers' hardness is 17GPa, and fracture toughness property is 7.41 MPam 1/2Its polished surface erosion profile as shown in Figure 2.
Embodiment 2
To add 5wt% sintering aid MgSiN 2The powder uniform mixing after, in the graphite jig of packing into then, SPS sintering under 30MPa, 1550 ℃, 12 minutes condition of soaking time.Sintering finishes the back sample and cools to room temperature with the furnace.
Silicon nitride ceramics thermal conductivity by above-mentioned prepared can reach 112W/mK, 3 folding strength σ bBe 800MPa, Vickers' hardness is 16.5GPa, and fracture toughness property is 7.68 MPam 1/2
Embodiment 3
To add 9wt% sintering aid MgSiN 2The powder uniform mixing after, in the graphite jig of packing into then, SPS sintering under 20MPa, 1550 ℃, 5 minutes condition of soaking time.Sintering finishes the back sample and cools to room temperature with the furnace.
Silicon nitride ceramics thermal conductivity by above-mentioned prepared can reach 63W/mK, 3 folding strength σ bBe 900MPa.
Embodiment 4
To add 5wt% sintering aid MgSiN 2The powder uniform mixing after, in the graphite jig of packing into then, SPS sintering under 80MPa, 1650 ℃, 30 minutes condition of soaking time.Sintering finishes the back sample and cools to room temperature with the furnace.
Silicon nitride ceramics thermal conductivity by above-mentioned prepared can reach 120W/mK, 3 folding strength σ bBe 798MPa.
Embodiment 5
To add 5wt% sintering aid BeSiN 2The powder uniform mixing after, in the graphite jig of packing into then, SPS sintering under 60MPa, 1600 ℃, 30 minutes condition of soaking time.Sintering finishes the back sample and cools to room temperature with the furnace.
Silicon nitride ceramics thermal conductivity by above-mentioned prepared can reach 95W/mK, 3 folding strength σ bBe 756MPa.
Embodiment 6
To add 5wt% sintering aid Mg 3N 2The powder uniform mixing after, in the graphite jig of packing into then, SPS sintering under 60MPa, 1600 ℃, 30 minutes condition of soaking time.Sintering finishes the back sample and cools to room temperature with the furnace.
Silicon nitride ceramics thermal conductivity by above-mentioned prepared can reach 85W/mK, 3 folding strength σ bBe 825MPa.
Embodiment 7
To add 5wt% sintering aid MgSiN 2, BeSiN 2And Mg 3N 2The powder uniform mixing after, in the graphite jig of packing into then, SPS sintering under 50MPa, 1650 ℃, 30 minutes condition of soaking time.Sintering finishes the back sample and cools to room temperature with the furnace.
Silicon nitride ceramics thermal conductivity by above-mentioned prepared can reach 103W/mK, 3 folding strength σ bBe 821MPa.
From above-mentioned seven embodiments as can be seen, the present invention adopts nitride as α-Si 3N 4The sintering aid of pottery preparation, and the method by SPS low temperature Fast Sintering have obtained the silicon nitride ceramics of high thermal conductance.

Claims (5)

1. a SiN ceramic with high heat conductivity preparation method is characterized in that
(a) with α-Si 3N 4Powder and be starting raw material as the nitride powder of sintering aid, both weight ratios are 100: 10～2; Described nitride is MgSiN 2, Mg 3N 2And BeSiN 2In any one, or their mixture;
(b) behind the powder uniform mixing that contains sintering aid with step (a), in the graphite jig of packing into, discharge plasma sintering under 10～100MPa, 1500～1700 ℃ condition;
(c) sintering cools to room temperature with the furnace after finishing.
2. by the described SiN ceramic with high heat conductivity preparation method of claim 1, it is characterized in that described α-Si 3N 4α phase weight percentage＞83% of powder, particle diameter are 0.3～10 μ m.
3. by the described SiN ceramic with high heat conductivity preparation method of claim 1, the purity that it is characterized in that described nitride as sintering aid is greater than 98%, and particle diameter is 0.3～10 μ m.
4. by the described SiN ceramic with high heat conductivity preparation method of claim 1, the soaking time that it is characterized in that discharge plasma sintering is 3～30 minutes.
5. by the described SiN ceramic with high heat conductivity preparation method of claim 1, it is characterized in that discharge plasma sintering carries out under vacuum or nitrogen.
CNB200610024154XA 2006-02-24 2006-02-24 Prepn process of SiN ceramic with high heat conductivity Expired - Fee Related CN100355701C (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN111085688A (en) * 2019-12-04 2020-05-01 西安交通大学 Tungsten/silicon nitride/tungsten symmetrical layered gradient composite material and rapid preparation method and application thereof

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CN101100388B (en) * 2007-07-17 2010-06-09 清华大学 High heat conductivity silicon nitride ceramics material and preparation method thereof
WO2010022789A1 (en) * 2008-08-29 2010-03-04 Ab Skf Method for manufacturing ceramic components
CN103086720A (en) * 2013-01-25 2013-05-08 西安交通大学 Rapid nitridation preparation method of silicon nitride-boron nitride composite ceramic though reactive sintering
CN103331420B (en) * 2013-06-20 2015-06-17 辽宁伊菲科技股份有限公司 High-nitrogen composite ceramic sprue cap for casting aluminum alloy
CN106747474B (en) * 2017-02-28 2020-05-08 安徽拓吉泰新型陶瓷科技有限公司 Preparation method of high-thermal-conductivity silicon nitride ceramic
CN108264345B (en) * 2018-02-01 2020-12-08 湖北工业大学 BaTiO3/CoFe2O4/BaTiO3Preparation method of nano multilayer composite magnetoelectric ceramic
CN109851369B (en) * 2019-01-24 2022-04-05 江西中科上宇科技有限公司 Method for preparing high-thermal-conductivity silicon nitride ceramic
CN110204343A (en) * 2019-04-19 2019-09-06 武汉理工大学 A kind of low temperature preparation method of high strength silicon nitride ceramics
CN111875387A (en) * 2020-06-24 2020-11-03 广东工业大学 Method for preparing silicon nitride ceramic with low oxygen content and high thermal conductivity by coating carbon and application thereof
CN115703683B (en) * 2021-08-17 2023-10-20 赛默肯(苏州)电子新材料有限公司 High-strength high-heat-conductivity large-size silicon nitride ceramic and preparation method thereof

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CN1537086A (en) * 2001-07-24 2004-10-13 ��ʽ���綫֥ Wear-resistance silicon nitride member and method for manufacturing thereof
CN1597614A (en) * 2004-05-17 2005-03-23 清华大学 Manufacturing method of high thermoconductivity high trength silicon nitride ceramic
CN1654427A (en) * 2005-01-14 2005-08-17 中国科学院上海硅酸盐研究所 Method for preparing high thermal conduction silicon nitride ceramic with magnesium silicon nitride as sintering aid

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Publication number Priority date Publication date Assignee Title
CN1537086A (en) * 2001-07-24 2004-10-13 ��ʽ���綫֥ Wear-resistance silicon nitride member and method for manufacturing thereof
CN1597614A (en) * 2004-05-17 2005-03-23 清华大学 Manufacturing method of high thermoconductivity high trength silicon nitride ceramic
CN1654427A (en) * 2005-01-14 2005-08-17 中国科学院上海硅酸盐研究所 Method for preparing high thermal conduction silicon nitride ceramic with magnesium silicon nitride as sintering aid

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN111085688A (en) * 2019-12-04 2020-05-01 西安交通大学 Tungsten/silicon nitride/tungsten symmetrical layered gradient composite material and rapid preparation method and application thereof
CN111085688B (en) * 2019-12-04 2021-08-13 西安交通大学 Tungsten/silicon nitride/tungsten symmetrical layered gradient composite material and rapid preparation method and application thereof

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