硅酸盐学报

Al2O3–RE2O3(RE=Lu, Y, Gd, La)烧结助剂对Si3N4陶瓷结构和性能的影响

作者：李天峰陈拥军李建保余辉李崴徐智超骆丽杰

单位：(海南大学材料与化工学院南海海洋资源利用国家重点实验室海口 570228)

关键词：氮化硅稀土氧化物微观结构力学性能

分类号：TQ174

出版年,卷(期):页码：2019,47(6):0-0

DOI：

摘要：

以α-Si3N4粉末为原料、Al2O3–RE2O3 (RE=Lu，Y，Gd和La)为烧结助剂，在1 800 ℃压烧结制备氮化硅陶瓷，研究了不同烧结助剂对材料的相组成、微观结构和力学性能的影响。结果表明：样品中α-Si3N4完全转化为β-Si3N4，所形成的长柱状晶粒生长发育良好。随着稀土阳离子半径的增大，材料的相对密度和力学性能呈增加趋势，其中Si3N4–Al2O3–Gd2O3的抗弯强度和断裂韧性分别达到860 MPa和7.2 MPa•m1/2。由于稀土离子对烧结液相黏度的影响，Si3N4–Al2O3–Lu2O3和Si3N4–Al2O3–Y2O3中出现了晶粒异常长大的现象，而Si3N4–Al2O3–La2O3的基体与柱状晶粒界面结合较大导致材料力学性能降低。

Silicon nitride ceramics were prepared via hot-pressing at a sintering temperature of 1800 ℃ with α-silicon nitride as a raw material and Al2O3–RE2O3 (RE=Lu, Y, Gd and La) as sintering additives. The effect of sintering additives on the phase composition, microstructure and mechanical properties of silicon nitride ceramics was investigated. The results show that α-Si3N4 in the sample can completely convert to β-Si3N4 with long columnar grains. The relative density and mechanical properties of the material increase with the increase of the rare-earth element ion radius, and the flexural strength and fracture toughness of Si3N4–Al2O3–Gd2O3 are 860 MPa and 7.2 MPa m1/2, respectively. Due to the effect of rare earth element ions on the viscosity of the sintered liquid phase, the growth of exaggerated grains occurs in the samples of Si3N4–Al2O3–Lu2O3 and Si3N4–Al2O3–Y2O3, and Si3N4–Al2O3–La2O3 has a strong grain interface bonding between the matrix and columnar grain , leading to the reduction of their mechanical properties.

基金项目：

国家自然科学基金(51702072)；国家高技术研发发展计划(863计划) (2015AA034103)。

作者简介：

参考文献：

[1] ZIEGLER A, IDROBO J C, CINIBULK M K, et al. Interface structure and atomic bonding characteristics in silicon nitride ceramics[J], Science, 2004, 306: 1768–1770.

[2] DAI J H, LI J B, CHEN Y J, et al. Effect of the residual phases in β-Si3N4 seed on the mechanical properties of self-reinforced Si3N4 ceramics[J]. J Eur Ceram Soc, 2003, 23(9): 1543–1547.

[3] BAL BS, KHANDKAR A, LAKSHMINARAYANAN R, et al. Fabrication and testing of silicon nitride bearings in total hip arthroplasty[J]. J Arthroplasty, 2009, 24(1): 110–116.

[4] WANG C M, PAN X Q, RUJLE M, et al. Silicon nitride crystal structure and observations of lattice defects[J]. J Mater Sci, 1996, 31: 5281–5298.

[5] NAOTO H, AKIRA O, KAZUO M. Sintering of Si3N4 with the addition of rare-earth oxides[J]. J Am Ceram Soc, 1988, 71(3): 365–372.

[6] KLEEBE H J, PEZZOTTI G, ZIEGLER G. Microstructure and fracture toughness of Si3N4 ceramics: combined roles of grain morphology and secondary phase chemistry[J]. J Am Ceram Soc, 1999, 82(7): 1857–1867.

[7] DAI J H, LI J B, CHEN Y J. The phase transformation behavior of Si3N4 with single Re2O3 (Re = Ce, Nd, Sm, Eu, Gd, Dy, Er, Yb) additive[J]. Mater Chem Phys, 2003, 80(1): 356–359.

[8] KITAYAMA M, HIRAO K, WATARI K, et al. Thermal conductivity of β-Si3N4: III, effect of rare-earth (RE= La, Nd, Gd, Y, Yb, and Sc) oxide additives[J]. J Am Ceram Soc, 2001, 84(2): 353–358.

[9] MELENDEZ-MARTINEZ J J, DOMINGUEZ-RODRIGUEZ A. Creep of silicon nitride[J]. Prog Mater Sci, 2004, 49(1): 19–107.

[10] SJIBATA N, PAINTER G S, SATET R L, et al. Rare-earth adsorption at intergranular interfaces in silicon nitride ceramics: subnanometer observations and theory[J]. Phys Rev B, 2005, 72(14): 140101(R).

[11] BECHER P F, PAINTER G S, SHIBATA N, et al. Effects of rare earth (RE) interganular adsorption on the phase transformation, microstructure evolution, and mechniacl properties in silicon nitride with RE2O3+MgO Additives: RE= La, Gd, and Lu[J]. J Am Ceram Soc, 2008, 91(7): 2328–2336.

[12] MIKIJELJ B, NAWAZ Z, KRUZIC J J, et al. Intergranular nanostructure effects on strength and toughness of Si3N4[J]. J Am Ceram Soc, 2015, 98(5): 1650–1657.

[13] ISO 14704-2016, Fine Ceramics (advanced ceramics, advanced technical ceramics)—test method for flexural strength of monolithic ceramics at room temperature[S]. Switzerland: ISO, 2016.

[14] AHMAD I, CAO H Z, CHEN H H, et al. Carbon nanotube toughened aluminium oxide nanocomposite[J]. J Eur Ceram Soc, 2010, 30(4): 865–873.

[15] HONMA T, UKYO Y. Sintering Process of Si3N4 with Y2O3 and Al2O3 as sintering additives[J]. J Mater Sci Lett, 1999, 18 (9): 735–737.

[16] BECHER P F, FERBER M K. Temperature-dependent viscosity of SiREAl-based glasses as a function of N: O and RE: Al ratios (RE=La, Gd, Y, and Lu)[J]. J Am Ceram Soc, 2004, 87(7): 1274–1279.

[17] SUN E Y, BECHER P F, PLUCKNETT K P, et al. Microstructural design of silicon nitride with improved fracture toughness: II, effects of yttria and alumina additives[J]. J Am Ceram Soc, 1998, 81(11): 2831–2840.

服务与反馈：

【文章下载】【加入收藏】