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Journal of Advanced Ceramics 2023, 12(1): 122-131 https://doi.org/10.26599/JAC.2023.9220671
Research Article | Open Access | Issue | Published: 23 December 2022

Design strategy of phase and microstructure of Si3N4 ceramics with simultaneously high hardness and toughness

Show Author's Information Shao-Jun TANGa,  Wei-Ming GUOa( ),  Shi-Kuan SUNb,  Hua-Tay LINa( )
School of Electromechanical Engineering, Guangdong University of Technology, Guangzhou 510006, China
School of Material Science and Energy Engineering, Foshan University, Foshan 528000, China
Keywords:
microstructure, hardness, toughness, phase composition, silicon nitride (Si3N4)
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TANG S-J, GUO W-M, SUN S-K, et al. Design strategy of phase and microstructure of Si3N4 ceramics with simultaneously high hardness and toughness. Journal of Advanced Ceramics, 2023, 12(1): 122-131. https://doi.org/10.26599/JAC.2023.9220671
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Abstract Full text About this article

Aiming to achieve silicon nitride (Si3N4) ceramics with high hardness and high toughness, the relationships among phase composition, microstructure, and mechanical properties of Si3N4 ceramics prepared by spark plasma sintering (SPS) at temperatures ranging from 1500 to 1800 ℃ were investigated in this study. Two stages with different phase and microstructure features were observed and summarized. The α–β phase transformation occurs first, and the development and growth of grains lag behind. During the first stage, the average grain size remains basically unchanged, and the hardness maintains at a value of ~20.18±0.26 GPa, despite the β-Si3N4 phase fraction increases from 7.67 to 57.34 wt%. Subsequently, the equiaxed grains transform into rod-like grains with a high aspect ratio via the reprecipitation process, resulting in a significant increase in the fracture toughness from 3.36±0.62 to 7.11±0.15 MPa·m1/2. In the second stage of sintering process, the fraction of β-Si3N4 phase increases to 100.00 wt%, and the grain growth also rapidly occurs. Thus, the fracture toughness increases slightly to 7.61±0.42 MPa·m1/2, but the hardness reduces to 16.80± 0.20 GPa. The current results demonstrate that the phase contents of β-Si3N4 and the microstructure shall be carefully tailored to achieve high-performance Si3N4 ceramics. Si3N4 ceramics with a fine-grained bimodal microstructure, consisting of the main α- and β-phases, can exhibit the optimized combination of hardness and toughness.


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About this article

Design strategy of phase and microstructure of Si3N4 ceramics with simultaneously high hardness and toughness

Show Author's information Shao-Jun TANGa, Wei-Ming GUOa( ), Shi-Kuan SUNb, Hua-Tay LINa( )
School of Electromechanical Engineering, Guangdong University of Technology, Guangzhou 510006, China
School of Material Science and Energy Engineering, Foshan University, Foshan 528000, China

Abstract

Aiming to achieve silicon nitride (Si3N4) ceramics with high hardness and high toughness, the relationships among phase composition, microstructure, and mechanical properties of Si3N4 ceramics prepared by spark plasma sintering (SPS) at temperatures ranging from 1500 to 1800 ℃ were investigated in this study. Two stages with different phase and microstructure features were observed and summarized. The α–β phase transformation occurs first, and the development and growth of grains lag behind. During the first stage, the average grain size remains basically unchanged, and the hardness maintains at a value of ~20.18±0.26 GPa, despite the β-Si3N4 phase fraction increases from 7.67 to 57.34 wt%. Subsequently, the equiaxed grains transform into rod-like grains with a high aspect ratio via the reprecipitation process, resulting in a significant increase in the fracture toughness from 3.36±0.62 to 7.11±0.15 MPa·m1/2. In the second stage of sintering process, the fraction of β-Si3N4 phase increases to 100.00 wt%, and the grain growth also rapidly occurs. Thus, the fracture toughness increases slightly to 7.61±0.42 MPa·m1/2, but the hardness reduces to 16.80± 0.20 GPa. The current results demonstrate that the phase contents of β-Si3N4 and the microstructure shall be carefully tailored to achieve high-performance Si3N4 ceramics. Si3N4 ceramics with a fine-grained bimodal microstructure, consisting of the main α- and β-phases, can exhibit the optimized combination of hardness and toughness.

Keywords: microstructure, hardness, toughness, phase composition, silicon nitride (Si3N4)

References(36)

[1]
Zhu XW, Sakka Y. Textured silicon nitride: Processing and anisotropic properties. Sci Technol Adv Mater 2008, 9: 033001.
DOI Google Scholar
[2]
Qin XW, Li S, Zhao L, et al. Silicon nitride ceramics consolidated by oscillatory pressure sintering. Ceram Int 2020, 46: 14235–14240.
DOI Google Scholar
[3]
Hou YB, Li B, Shao CW, et al. Effect of high-temperature annealing in air and N2 atmosphere on the mechanical properties of Si3N4 fibers. Mater Sci Eng A 2018, 724: 502–508.
DOI Google Scholar
[4]
Xu SS, Zhou XN, Zhi Q, et al. Anisotropic, biomorphic cellular Si3N4 ceramics with directional well-aligned nanowhisker arrays based on wood-mimetic architectures. J Adv Ceram 2022, 11: 656–664.
DOI Google Scholar
[5]
Dang XL, Zhao DL, Guo T, et al. Oxidation behaviors of carbon fiber reinforced multilayer SiC–Si3N4 matrix composites. J Adv Ceram 2022, 11: 354–364.
DOI Google Scholar
[6]
Petzow G, Herrmann M. Silicon nitride ceramics. In: High Performance Non-oxide Ceramics II. Structure and Bonding. Jansen M, Ed. Berlin: Springer Berlin Heidelberg, 2002, 102: 47–167.
DOI
[7]
Greskovich C, Gazza GE. Hardness of dense α- and β-Si3N4 ceramics. J Mater Sci Lett 1985, 4: 195–196.
DOI Google Scholar
[8]
Ziegler G, Heinrich J, Wötting G. Relationships between processing, microstructure and properties of dense and reaction-bonded silicon nitride. J Mater Sci 1987, 22: 3041–3086.
DOI Google Scholar
[9]
Kawaoka H, Adachi T, Sekino T, et al. Effect of α/β phase ratio on microstructure and mechanical properties of silicon nitride ceramics. J Mater Res 2001, 16: 2264–2270.
DOI Google Scholar
[10]
Kong JH, Ma HJ, Jung WK, et al. Self-reinforced and high-thermal conductivity silicon nitride by tailoring α–β phase ratio with pressureless multi-step sintering. Ceram Int 2021, 47: 13057–13064.
DOI Google Scholar
[11]
Ziegler A, McNaney JM, Hoffmann MJ, et al. On the effect of local grain-boundary chemistry on the macroscopic mechanical properties of a high-purity Y2O3–Al2O3-containing silicon nitride ceramic: Role of oxygen. J Am Ceram Soc 2005, 88: 1900–1908.
DOI Google Scholar
[12]
Lee CJ, Chae JI, Kim DJ. Effect of β-Si3N4 starting powder size on elongated grain growth in β-Si3N4 ceramics. J Eur Ceram Soc 2000, 20: 2667–2671.
DOI Google Scholar
[13]
Hirao K, Nagaoka T, Brito ME, et al. Microstructure control of silicon nitride by seeding with rodlike β-silicon nitride particles. J Am Ceram Soc 1994, 77: 1857–1862.
DOI Google Scholar
[14]
Dai JH, Li JB, Chen YJ, et al. Effect of the residual phases in β-Si3N4 seed on the mechanical properties of self-reinforced Si3N4 ceramics. J Eur Ceram Soc 2003, 23: 1543–1547.
DOI Google Scholar
[15]
De Pablos A, Osendi MI, Miranzo P. Correlation between microstructure and toughness of hot pressed Si3N4 ceramics seeded with β-Si3N4 particles. Ceram Int 2003, 29: 757–764.
DOI Google Scholar
[16]
Hyuga H, Jones MI, Hirao K, et al. Influence of rare-earth additives on wear properties of hot-pressed silicon nitride ceramics under dry sliding conditions. J Am Ceram Soc 2004, 87: 1683–1686.
DOI Google Scholar
[17]
Pigeon RG, Varma A. Quantitative phase analysis of Si3N4 by X-ray diffraction. J Mater Sci Lett 1992, 11: 1370–1372.
DOI Google Scholar
[18]
Fu L, Engqvist H, Xia W. Spark plasma sintering of biodegradable Si3N4 bioceramic with Sr, Mg and Si as sintering additives for spinal fusion. J Eur Ceram Soc 2018, 38: 2110–2119.
DOI Google Scholar
[19]
Evans AG, Charles EA. Fracture toughness determinations by indentation. J Am Ceram Soc 1976, 59: 371–372.
DOI Google Scholar
[20]
Hampshire S, Pomeroy MJ. Grain boundary glasses in silicon nitride: A review of chemistry, properties and crystallisation. J Eur Ceram Soc 2012, 32: 1925–1932.
DOI Google Scholar
[21]
Nishimura T, Mitomo M, Hirotsuru H, et al. Fabrication of silicon nitride nano-ceramics by spark plasma sintering. J Mater Sci Lett 1995, 14: 1046–1047.
DOI Google Scholar
[22]
Suganuma M, Kitagawa Y, Wada S, et al. Pulsed electric current sintering of silicon nitride. J Am Ceram Soc 2003, 86: 387–394.
DOI Google Scholar
[23]
Belmonte M, González-Julián J, Miranzo P, et al. Spark plasma sintering: A powerful tool to develop new silicon nitride-based materials. J Eur Ceram Soc 2010, 30: 2937–2946.
DOI Google Scholar
[24]
Hampshire S. Silicon nitride ceramics—Review of structure, processing and properties. J Achiev Mater Manuf Eng 2007, 24: 43–50.
Google Scholar
[25]
Kitayama M, Hirao K, Toriyama M, et al. Modeling and simulation of grain growth in Si3N4—II. The α–β transformation. Acta Mater 1998, 46: 6551–6557.
DOI Google Scholar
[26]
Bahrami S, Zakeri M, Faeghinia A, et al. Effect of the alfa content on the mechanical properties of Si3N4/BAS composite by spark plasma sintering. J Alloys Compd 2018, 756: 76–81.
DOI Google Scholar
[27]
Tatarková M, Tatarko P, Šajgalík P. Si3N4 ceramics, structure and properties. In: Encyclopedia of Materials: Technical Ceramics and Glasses. Pomeroy M, Ed. Amsterdam, the Netherlands: Elsevier Amsterdam, 2021, 2: 109–118.
DOI
[28]
Tatarko P, Lojanová Š, Dusza J, et al. Influence of various rare-earth oxide additives on microstructure and mechanical properties of silicon nitride based nanocomposites. Mater Sci Eng A 2010, 527: 4771–4778.
DOI Google Scholar
[29]
Šajgalík P, Dusza J, Hoffmann MJ. Relationship between microstructure, toughening mechanisms, and fracture toughness of reinforced silicon nitride ceramics. J Am Ceram Soc 1995, 78: 2619–2624.
DOI Google Scholar
[30]
Satet RL, Hoffmann MJ, Cannon RM. Experimental evidence of the impact of rare-earth elements on particle growth and mechanical behaviour of silicon nitride. Mater Sci Eng A 2006, 422: 66–76.
DOI Google Scholar
[31]
Šajgalík P, Galusek D. α/β Phase transformation of silicon nitride: Homogeneous and heterogeneous nucleation. J Mater Sci Lett 1993, 12: 1937–1939.
DOI Google Scholar
[32]
Krämer M, Wittmüss D, Küppers H, et al. Relations between crystal structure and growth morphology of β-Si3N4. J Cryst Growth 1994, 140: 157–166.
DOI Google Scholar
[33]
Lai KR, Tien TY. Kinetics of β-Si3N4 grain growth in Si3N4 ceramics sintered under high nitrogen pressure. J Am Ceram Soc 1993, 76: 91–96.
DOI Google Scholar
[34]
Peng GH, Li XG, Liang M, et al. Spark plasma sintered high hardness α/β Si3N4 composites with MgSiN2 as additives. Scr Mater 2009, 61: 347–350.
DOI Google Scholar
[35]
Kitayama M, Hirao K, Toriyama M, et al. Modeling and simulation of grain growth in Si3N4—I. Anisotropic Ostwald ripening. Acta Mater 1998, 46: 6541–6550.
DOI Google Scholar
[36]
Tan DW, Zhu LL, Wei WX, et al. Performance improvement of Si3N4 ceramic cutting tools by tailoring of phase composition and microstructure. Ceram Int 2020, 46: 26182–26189.
DOI Google Scholar
Publication history
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Publication history

Received: 11 July 2022
Revised: 30 September 2022
Accepted: 01 October 2022
Published: 23 December 2022
Issue date: January 2023

Copyright

© The Author(s) 2022.

Acknowledgements

This work was supported by the Shandong Provincial Key Research and Development Program (2019JZZY010330), the National Natural Science Foundation of China (52172066 and 52172064), the Key Research and Development Project of Gansu Province (21YF5WA140), and the Science and Technology Program of Guangzhou (201704030095). Shi-Kuan Sun acknowledges the Guangdong Key Platform & Programs of the Education Department of Guangdong Province (2021ZDZX1003) and the Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure (SKL202104SIC).

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