Al_2O_3–RE_2O_3(RE=Lu,Y,Gd,La)烧结助剂对Si_3N_4陶瓷结构和性能的影响
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摘要
以α-Si_3N_4粉末为原料、Al_2O_3–RE_2O_3(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-Si_3N_4完全转化为β-Si_3N_4,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Si_3N_4–Al_2O_3–Gd_2O_3的抗弯强度和断裂韧性分别达到860 MPa和7.2 MPa·m~(1/2)。由于稀土离子对烧结液相黏度的影响,Si_3N_4–Al_2O_3–Lu_2O_3和Si_3N_4–Al_2O_3–Y_2O_3中出现了晶粒异常长大的现象,而Si_3N_4–Al_2O_3–La_2O_3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℃withα-silicon nitride as a raw material and Al_2O_3–RE_2O_3(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 thatα-Si_3N_4 in the sample can completely convert toβ-Si_3N_4 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 Si_3N_4–Al_2O_3–Gd_2O_3 are 860MPa and 7.2 MPa m~(1/2),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 Si_3N_4–Al_2O_3–Lu_2O_(3 )and Si_3N_4–Al_2O_3–Y_2O_3,and Si_3N_4–Al_2O_3–La_2O_3 has a strong grain interface bonding between the matrix and columnar grain,leading to the reduction of their mechanical properties.
Silicon nitride ceramics were prepared via hot-pressing at a sintering temperature of 1800℃withα-silicon nitride as a raw material and Al_2O_3–RE_2O_3(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 thatα-Si_3N_4 in the sample can completely convert toβ-Si_3N_4 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 Si_3N_4–Al_2O_3–Gd_2O_3 are 860MPa and 7.2 MPa m~(1/2),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 Si_3N_4–Al_2O_3–Lu_2O_(3 )and Si_3N_4–Al_2O_3–Y_2O_3,and Si_3N_4–Al_2O_3–La_2O_3 has a strong grain interface bonding between the matrix and columnar grain,leading to the reduction of their mechanical properties.
引文
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[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.
[2]DAI J H,LI J B,CHEN Y J,et al.Effect of the residual phases inβ-Si3N4 seed on the mechanical properties of self-reinforced Si3N4ceramics[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 ofβ-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.
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