Preparation and properties of spodumene/silicon carbide composite ceramic materials

Lu Yuan-Yuan; Lu Gui-Hua; Zhou Heng-Wei; Huang Yi-Neng

doi:10.7498/aps.69.20200232

Abstract

Silicon carbide (SiC) is widely used due to the lower coefficient of thermal expansion (CTE), high thermal conductivity and excellent mechanical properties. However, the self-diffusion coefficient of SiC relative to that of oxide ceramics is very low, it is difficult to sinter at lower temperature. The β-spodumene has ultra low or even negative thermal expansion coefficient combined with good thermal and chemical durability, which melts at 1423 ℃. Accordingly, the present study focuses on the use of β-spodumene as a flux at lower sintering temperature and the preparation of lower CET composite ceramics. The effects of spodumene on the sintering behavior, phase relations, thermal expansion and mechanical properties of spodumene/silicon carbide composites are discussed.A high pure β-spodumene LiAlSi₂O₆ compound with nearly zero thermal expansion coefficient is synthesized via solid phase sintering. Spodumene/silicon carbide composites are fabricated by the adding 25, 30, 35 and 40 mass% synthesized β-spodumene powder to 75, 70, 65 and 60 mass% α-SiC matrix, respectively. Both β-spodumene and SiC are fabricated by conventional pressureless liquid sintering technique, and the batches are uniaxially pressed into discs and rectangular bars, then sintered at 1550 ℃ for 2 h in an Ar atmosphere.The results show that the SiC and β-spodumene do not react during sintering, and the β-spodumene changes from tetragonal phase into hexagonal phase, the cell volume has a considerable shrinkage. A certain amount of liquid phase can help to enhance the density, improve Young’s modulus and promote the sintering behavior of SiC. When the feedstock contains 35% β-spodumene, the Young’s modulus reaches to (204.2 ± 0.5) GPa. Excess porosity is formed when liquid phase is too much during sintering, The Young's modulus of the sample 40SP is (119.6 ± 0.5) GPa. It is determined that the Young’s modulus of these materials are affected by porosity and internal microcracks. This study indicates that the content of β-spodumene and porosity are the dominant factors to control the CET of composites, but the porosity has a stronger effect. Besides, the microcracks, which are formed by the interaction of various internal stresses, are also an impotant factor. The materials with nearly zero thermal expansion are developed in a lower temperature range from –150 ℃ to 25 ℃, the spodumene content in the most stable composite reaches 40 mass%, and the CET of composite is close to that of Si (α_{25 ℃} = 2.59 × 10^–6 ℃^–1) in a temperature range of 25–480 ℃.

Keywords:

Authors and contacts

1.
Xinjiang Laboratory of Phase Transitions and Microstructures in Condensed Matters, College of Physical Science and Technology, Yili Normal University, Yining 835000, China
2.
National Laboratory of Solid State Microstructures, School of Physics, Nanjing University, Nanjing 210093, China

Corresponding author: Zhou Heng-Wei, zhw33221@163.com ; Huang Yi-Neng, ynhuang@nju.edu.cn

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References

[1]	Mandal S, Chakrabarti S, Das S K, Ghatak S 2007 Ceram. Int. 33 123 Google Scholar
[2]	Abdel-Fattah W I, Abdellah R 1997 Ceram. Int. 23 463 Google Scholar
[3]	Hummel F A 1951 J. Am. Ceram. Soc. 34 235 Google Scholar
[4]	Roy R, Agrawal D K, Mckinstry H A 2003 Annu. Rev. Mater. Res. 19 59 Google Scholar
[5]	Ramirez I J, Matsumaru K, Ishizaki K 2006 J. Ceram. Soc. Jpn. 114 1111 Google Scholar
[6]	Ono T, Matsumaru K, Juárez-Ramírez I, Torres-Martínez L M, Ishizaki K 2009 Mater. Sci. Forum 620–622 715 Google Scholar
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[8]	García-Moreno O, Fernández A, Torrecillas R 2010 J. Eur. Ceram. Soc. 30 3219 Google Scholar
[9]	Iwashima M, Nakano H, Ogata T O, Tsurumi T, Urabe K 2003 J. Ceram. Soc. Jpn. 111 430 Google Scholar
[10]	Iguchi M, Umezu M, Kataoka M, Nakamura H, Ishii M 2006 Key Eng. Mater. 317-318 177 Google Scholar
[11]	Welsch A M, Murawski D, Prekajski M, Vulic P, Kremenovic A 2015 Phys. Chem. Miner. 42 413 Google Scholar
[12]	Li C T 1968 Z. Kristallogr. Kristallgeom. Kristallphys. Kristallchem. 127 327 Google Scholar
[13]	Ostertag W, Fischer G R, Williams J P 1968 J. Am. Ceram. Soc. 51 651 Google Scholar
[14]	Manurung P, Low I M, O’Connor B H, Kennedy S 2005 Mater. Res. Bull. 40 2047 Google Scholar
[15]	曹爱红 2006 中国陶瓷 42 30 Google Scholar Cao A H 2006 Chn. Ceram. 42 30 Google Scholar
[16]	Awaad M, Mӧrtel H, Naga S M 2005 J. Mater. Sci. -Mater. Electron. 16 377 Google Scholar
[17]	Bayuseno A P, Latella B A, O'Connor B H 1999 J. Am. Ceram. Soc. 82 819 Google Scholar
[18]	Latella B A, Burton G R, O'Connort B H 1995 J. Am. Ceram. Soc. 78 1895 Google Scholar
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[25]	吴清仁, 吴建青, 文壁璇 1994 94'全国结构陶瓷、功能陶瓷、金属/陶瓷封接学术会议论文集 (中国北京) 10月20—24日 1994 p174 Wu Q R, Wu J Q, Wen B X 1994 Proceedings of the 94' National symposium on Structural Ceramics, Functional Ceramics, Metal/Ceramic Sealing Beijing, China, October 20–24, 1994 p174 (in Chinese)
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[28]	Li C T 1970 Z. Kristallogr. Kristallgeom. Kristallphys. Kristallchem. 132 118 Google Scholar
[29]	Kobayashi H, Ishibashi N, Akiba T, Mitamura T 1990 J. Ceram. Soc. Jpn. 98 1023 Google Scholar
[30]	Xia L, Wang X Y, Wen G W, Zhong B, Song L 2012 Ceram. Int. 38 5315 Google Scholar
[31]	Okada Y, Tokumaru Y 1984 J. Appl. Phys. 56 314 Google Scholar
[32]	喻佑华, 刘映珍 1995 陶瓷研究 10 180 Yu Y H, Liu Y Z 1995 Ceram. Stud. J. 10 180

Cited By

图 1 β-锂辉石XRD图谱　(a) β-LiAlSi₂O₆; (b) ICSD No. 01-071-2058

Figure 1. XRD patterns of β-spodumene: (a) β-LiAlSi₂O₆; (b) ICSD No. 01-071-2058

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图 2 锂辉石/碳化硅复相陶瓷XRD图谱

Figure 2. XRD patterns of spodumene/silicon carbide composi-tes.

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图 3 1550 ℃烧结前后试样40SP的XRD图谱

Figure 3. XRD patterns of 40SP sample in the starting and the sintered at 1550 ℃.

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图 4 锂辉石/碳化硅复相陶瓷断面显微形貌　(a) 25SP; (b) 30SP; (c) 35SP; (d) 40SP

Figure 4. SEM micrographs of the fracture surface of spodumene/silicon composites: (a) 25SP; (b) 30SP; (c) 35SP; (d) 40SP.

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图 5 锂辉石/碳化硅复相陶瓷的气孔率和杨氏模量

Figure 5. Apparent porosity and Young’s modulus of the spodumene/silicon carbide composites.

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图 6 锂辉石/碳化硅复相陶瓷热膨胀率随温度的变化关系

Figure 6. Expansion versus temperature of the spodumene/sili-con carbide composites.

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图 7 35 SP复相陶瓷的微裂纹

Figure 7. Microcrack of 35 SP composite.

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表 1 LAS体系一些重要物质的平均线热膨胀系数

Table 1. Average linear thermal expansion coefficient (CET) of some important materials based on LAS system.

System/material	CET/10^–6 ℃^–1	Temperature range/℃
Li₂O·Al₂O₃·2SiO₂ (LiAlSiO₄, Eucryptite)	–6.2	25—800
Li₂O·Al₂O₃·3SiO₂ (Solid solution of eucryptite)	Negative near zero CET	25—1000
Li₂O·Al₂O₃·4SiO₂ (β-LiAlSi₂O₆, β-Spodumene)	0.9	25—1000
Li₂O·Al₂O₃·6SiO₂ (LiAlSi₃O₈, Virgilite)	0.5	25—1000
Li₂O·Al₂O₃·8SiO₂ (LiAlSi₄O₁₀, Petalite)	0.3	25—1000
Li₂O·Al₂O₃·10SiO₂	0.5	25—1000
LAS + TiO₂ (Pyroceram)	–0.07—0.30
LAS + TiO₂ + ZrO₂ (Cer-Vit)	0.05—0.30
Hercuvit (LAS-based transparentlow expanding glass-ceramic)	0—0.3

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表 2 四方相β-锂辉石和六方相锂辉石原子键长、晶胞体积和密度

Table 2. The atomic bond lengths, cell volume and density of tetragonal and hexagonal spodumene.

Phase	Si, Al—O/Å	Li—O/ Å	Si, Al—Li/Å	O—O (Li tetrahedra)/Å	O—O (Si, Al tetrahedra)/Å	V/Å³	D_c/g·cm^–3
Te-SP	1.643	2.081	2.628/2.710	3.339	2.682	520.671	2.374
He-SP	1.641	2.068	2.609	3.337	2.679	128.790	2.399

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表 3 锂辉石/碳化硅复相陶瓷材料的性能

Table 3. Characteristics of spodumene/ silicon carbide composites.

β–Spodumene content/ mass%	Apparent porosity/ %	Bulk density/ g·cm^–3	Young’s modulus/ GPa	α (–150—25 ℃)/ ℃^–1	α (25—480 ℃)/ ℃^–1
SP25	38	1.81	95.3 ± 0.1	0.23 × 10^–6	1.83 × 10^–6
SP30	32	1.82	123.8 ± 0.4	0.60 × 10^–6	2.95 × 10^–6
SP35	19	2.24	204.2 ± 0.5	0.53 × 10^–6	5.71 × 10^–6
SP40	29	1.95	119.6 ± 0.5	1.14 × 10^–6	2.50 × 10^–6

DownLoad: CSV

[1]	Mandal S, Chakrabarti S, Das S K, Ghatak S 2007 Ceram. Int. 33 123 Google Scholar
[2]	Abdel-Fattah W I, Abdellah R 1997 Ceram. Int. 23 463 Google Scholar
[3]	Hummel F A 1951 J. Am. Ceram. Soc. 34 235 Google Scholar
[4]	Roy R, Agrawal D K, Mckinstry H A 2003 Annu. Rev. Mater. Res. 19 59 Google Scholar
[5]	Ramirez I J, Matsumaru K, Ishizaki K 2006 J. Ceram. Soc. Jpn. 114 1111 Google Scholar
[6]	Ono T, Matsumaru K, Juárez-Ramírez I, Torres-Martínez L M, Ishizaki K 2009 Mater. Sci. Forum 620–622 715 Google Scholar
[7]	Wang B, Yang X H, Zeng D J, Yang J F, Ishizaki K, Niihara K 2014 J. Eur. Ceram. Soc. 34 97 Google Scholar
[8]	García-Moreno O, Fernández A, Torrecillas R 2010 J. Eur. Ceram. Soc. 30 3219 Google Scholar
[9]	Iwashima M, Nakano H, Ogata T O, Tsurumi T, Urabe K 2003 J. Ceram. Soc. Jpn. 111 430 Google Scholar
[10]	Iguchi M, Umezu M, Kataoka M, Nakamura H, Ishii M 2006 Key Eng. Mater. 317-318 177 Google Scholar
[11]	Welsch A M, Murawski D, Prekajski M, Vulic P, Kremenovic A 2015 Phys. Chem. Miner. 42 413 Google Scholar
[12]	Li C T 1968 Z. Kristallogr. Kristallgeom. Kristallphys. Kristallchem. 127 327 Google Scholar
[13]	Ostertag W, Fischer G R, Williams J P 1968 J. Am. Ceram. Soc. 51 651 Google Scholar
[14]	Manurung P, Low I M, O’Connor B H, Kennedy S 2005 Mater. Res. Bull. 40 2047 Google Scholar
[15]	曹爱红 2006 中国陶瓷 42 30 Google Scholar Cao A H 2006 Chn. Ceram. 42 30 Google Scholar
[16]	Awaad M, Mӧrtel H, Naga S M 2005 J. Mater. Sci. -Mater. Electron. 16 377 Google Scholar
[17]	Bayuseno A P, Latella B A, O'Connor B H 1999 J. Am. Ceram. Soc. 82 819 Google Scholar
[18]	Latella B A, Burton G R, O'Connort B H 1995 J. Am. Ceram. Soc. 78 1895 Google Scholar
[19]	Naga S M, El-Maghraby A A, Hassan A M 2016 Ceram. Int. 42 12161 Google Scholar
[20]	Low I M, Mathews E, Garrod T, Zhou D, Phillip D N, Pillai X M 1997 J. Mater. Sci. 32 3807 Google Scholar
[21]	Shi C G, Low I M 1998 Mater. Lett. 36 118 Google Scholar
[22]	Halbig M C, Singh M, Tsuda H 2012 Int. J. Appl. Ceram. Technol. 9 677 Google Scholar
[23]	赵赞良, 唐政维, 蔡雪梅, 李秋俊, 张宪力 2006 装备制造技术 4 81 Google Scholar Zhao Z L, Tang Z W, Cai X M, Li Q J, Zhang X L 2006 Equip. Manuf. Technol. 4 81 Google Scholar
[24]	赵更一 2016 硕士学位论文 (黑龙江: 哈尔滨工业大学) Zhao G Y 2016 M.S. Thesis (Harbin: Harbin Institute of Technology) (in Chinese)
[25]	吴清仁, 吴建青, 文壁璇 1994 94'全国结构陶瓷、功能陶瓷、金属/陶瓷封接学术会议论文集 (中国北京) 10月20—24日 1994 p174 Wu Q R, Wu J Q, Wen B X 1994 Proceedings of the 94' National symposium on Structural Ceramics, Functional Ceramics, Metal/Ceramic Sealing Beijing, China, October 20–24, 1994 p174 (in Chinese)
[26]	黄智恒, 贾德昌, 杨治华, 周玉 2004 材料科学与工艺 12 103 Google Scholar Huang Z H, Jia D C, Yang Z H, Zhou Y 2004 Mater. Sci. Technol. 12 103 Google Scholar
[27]	Liang H Q, Yao X M, Liu X J, Huang Z R 2014 Mater. Des. 56 1009 Google Scholar
[28]	Li C T 1970 Z. Kristallogr. Kristallgeom. Kristallphys. Kristallchem. 132 118 Google Scholar
[29]	Kobayashi H, Ishibashi N, Akiba T, Mitamura T 1990 J. Ceram. Soc. Jpn. 98 1023 Google Scholar
[30]	Xia L, Wang X Y, Wen G W, Zhong B, Song L 2012 Ceram. Int. 38 5315 Google Scholar
[31]	Okada Y, Tokumaru Y 1984 J. Appl. Phys. 56 314 Google Scholar
[32]	喻佑华, 刘映珍 1995 陶瓷研究 10 180 Yu Y H, Liu Y Z 1995 Ceram. Stud. J. 10 180

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