Effect of Ternary Composite Sintering Agent Er2O3-Mg2Si-Yb2O3 on Properties of Silicon Nitride Ceramics

Abstract

Abstract: High thermal conductivity Si₃N₄ ceramics with excellent mechanical properties were prepared by using ternary composite sintering agent Er₂O₃-Mg₂Si-Yb₂O₃. The effects of Er₂O₃-Mg₂Si-Yb₂O₃ system on densification, microstructure, mechanical properties and thermal conductivity of Si₃N₄ ceramics were studied. The results show that when the sintering agent is 5% (mass fraction, the same below) Er₂O₃+2%Mg₂Si+4%Yb₂O₃, the effect of sintering agent on the balance between density and the content of grain boundary phase of Si₃N₄ ceramics is the best. At the moment, Si₃N₄ ceramics have the best properties, such as bending strength of 765 MPa, fracture toughness of 7.2 MPa·m^1/2, and thermal conductivity of 67 W/(m·K). In the sintering process, adding only 5%Er₂O₃+2%Mg₂Si produces less liquid phase with high viscosity, which cannot densify the Si₃N₄ ceramics. When the content of Yb₂O₃ exceeds 4%, the sintering agent produces a large amount of grain boundary phase, which reduces the properties of Si₃N₄ ceramics.

Key words: silicon nitride ceramics, Er₂O₃-Mg₂Si-Yb₂O₃ sintering agent, density, microstructure, mechanical property, thermal conductivity

CLC Number:

TQ174.75

JIANG Changxi, ZHOU Lijuan, ZHUANG Yinghua, LIAO Shengjun, WANG Jianjun. Effect of Ternary Composite Sintering Agent Er₂O₃-Mg₂Si-Yb₂O₃ on Properties of Silicon Nitride Ceramics[J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(4): 1423-1432.

References

[1] HU F, XIE Z P, ZHANG J, et al. Promising high-thermal-conductivity substrate material for high-power electronic device: silicon nitride ceramics[J]. Rare Metals, 2020, 39(5): 463-478.
[2] WANG W D, YAO D X, LIANG H Q, et al. Effect of in situ formed Y₂O₃ by metal hydride reduction reaction on thermal conductivity of β-Si₃N₄ ceramics[J]. Journal of the European Ceramic Society, 2020, 40(15): 5316-5323.
[3] PARK Y J, PARK M J, KIM J M, et al. Sintered reaction-bonded silicon nitrides with high thermal conductivity: the effect of the starting Si powder and Si₃N₄ diluents[J]. Journal of the European Ceramic Society, 2014, 34(5): 1105-1113.
[4] GOLLA B R, KO J W, KIM J M, et al. Effect of particle size and oxygen content of Si on processing, microstructure and thermal conductivity of sintered reaction bonded Si₃N₄[J]. Journal of Alloys and Compounds, 2014, 595: 60-66.
[5] ZHOU Y, HYUGA H, KUSANO D, et al. Effects of yttria and magnesia on densification and thermal conductivity of sintered reaction-bonded silicon nitrides[J]. Journal of the American Ceramic Society, 2019, 102(4): 1579-1588.
[6] ZHU X W, SAKKA Y, ZHOU Y, et al. A strategy for fabricating textured silicon nitride with enhanced thermal conductivity[J]. Journal of the European Ceramic Society, 2014, 34(10): 2585-2589.
[7] LU H, BAILEY C, YIN C Y. Design for reliability of power electronics modules[J]. Microelectronics Reliability, 2009, 49(9/10/11): 1250-1255.
[8] BUTTAY C, PLANSON D, ALLARD B, et al. State of the art of high temperature power electronics[J]. Materials Science and Engineering: B, 2011, 176(4): 283-288.
[9] MURAYAMA N, HIRAO K, SANDO M, et al. High-temperature electro-ceramics and their application to SiC power modules[J]. Ceramics International, 2018, 44(4): 3523-3530.
[10] HIROSAKI N, OGATA S, KOCER C, et al. Molecular dynamics calculation of the ideal thermal conductivity of single-crystal α- and β-Si₃N₄[J]. Physical Review B, 2002, 65(13): 134110.
[11] HAYASHI H, HIRAO K, KITAYAMA M, et al. Effect of oxygen content on thermal conductivity of sintered silicon nitride[J]. Journal of the Ceramic Society of Japan, 2001, 109(1276): 1046-1050.
[12] ZHOU Y, HYUGA H, KUSANO D, et al. A tough silicon nitride ceramic with high thermal conductivity[J]. Advanced Materials (Deerfield Beach, Fla), 2011, 23(39): 4563-4567.
[13] WANG W D, YAO D X, LIANG H Q, et al. Improved thermal conductivity of β-Si₃N₄ ceramics through the modification of the liquid phase by using GdH₂ as a sintering additive[J]. Ceramics International, 2021, 47(4): 5631-5638.
[14] WANG W D, YAO D X, LIANG H Q, et al. Enhanced thermal conductivity in Si₃N₄ ceramics prepared by using ZrH₂ as an oxygen getter[J]. Journal of Alloys and Compounds, 2021, 855: 157451.
[15] WANG W D, YAO D X, CHEN H B, et al. ZrSi₂-MgO as novel additives for high thermal conductivity of β-Si₃N₄ ceramics[J]. Journal of the American Ceramic Society, 2020, 103(3): 2090-2100.
[16] WANG W D, YAO D X, LIANG H Q, et al. Effect of the binary nonoxide additives on the densification behavior and thermal conductivity of Si₃N₄ ceramics[J]. Journal of the American Ceramic Society, 2020, 103(10): 5891-5899.
[17] LUO J, LI J G, LI M J, et al. Low-temperature densification by plasma activated sintering of Mg₂Si-added Si₃N₄[J]. Ceramics International, 2019, 45(12): 15128-15133.
[18] LIU W, TONG W X, LU X X, et al. Effects of different types of rare earth oxide additives on the properties of silicon nitride ceramic substrates[J]. Ceramics International, 2019, 45(9): 12436-12442.
[19] 杨亮亮,谢志鹏,宋明.Yb₂O₃-Al₂O₃烧结助剂对气压烧结氮化硅陶瓷性能的影响[J].人工晶体学报,2016,45(1):104-109.
YANG L L, XIE Z P, SONG M. Effect of Yb₂O₃-Al₂O₃ sintering aids on the properties of silicon nitride ceramics prepared by gas pressure sintering[J]. Journal of Synthetic Crystals, 2016, 45(1): 104-109 (in Chinese).
[20] DUAN Y S, LIU N, ZHANG J X, et al. Cost effective preparation of Si₃N₄ ceramics with improved thermal conductivity and mechanical properties[J]. Journal of the European Ceramic Society, 2020, 40(2): 298-304.
[21] GUO W M, WU L X, MA T, et al. Rapid fabrication of Si₃N₄ ceramics by reaction-bonding and pressureless sintering[J]. Journal of the European Ceramic Society, 2016, 36(16): 3919-3924.
[22] MENG Q Y, ZHAO Z H, SUN Y Q, et al. Low temperature pressureless sintering of dense silicon nitride using BaO-Al₂O₃-SiO₂ glass as sintering aid[J]. Ceramics International, 2017, 43(13): 10123-10129.
[23] 刘剑,谢志鹏,肖志才,等.烧结助剂对氮化硅陶瓷热导率和力学性能的影响[J].硅酸盐学报,2020,48(12):1865-1871.
LIU J, XIE Z P, XIAO Z C, et al. Effect of sintering aids on thermal conductivity and mechanical properties of silicon nitride ceramics[J]. Journal of the Chinese Ceramic Society, 2020, 48(12): 1865-1871 (in Chinese).
[24] YE C C, JIANG Y, YUE X Y, et al. Effect of temperature and pre-sintering on phase transformation, texture and mechanical properties of silicon nitride ceramics[J]. Materials Science and Engineering: A, 2018, 731: 140-148.
[25] HAMPSHIRE S, POMEROY M J. Grain boundary glasses in silicon nitride: a review of chemistry, properties and crystallisation[J]. Journal of the European Ceramic Society, 2012, 32(9): 1925-1932.
[26] BALANDIN A, WANG K L. Significant decrease of the lattice thermal conductivity due to phonon confinement in a free-standing semiconductor quantum well[J]. Physical Review B, 1998, 58(3): 1544-1549.
[27] YANG P, XU F H, LI J B, et al. The impact of oxygen impurity and La doping on thermodynamic properties of Si₃N₄ ceramic: a first-principle calculation approach[J]. Journal of the European Ceramic Society, 2020, 40(15): 5293-5297.
[28] LIAO S J, ZHOU L J, JIANG C X, et al. Thermal conductivity and mechanical properties of Si₃N₄ ceramics with binary fluoride sintering additives[J]. Journal of the European Ceramic Society, 2021, 41(14): 6971-6982.
[29] LI Y S, KIM H N, WU H B, et al. Microstructure and thermal conductivity of gas-pressure-sintered Si₃N₄ ceramic: the effects of Y₂O₃ additive content[J]. Journal of the European Ceramic Society, 2021, 41(1): 274-283.
[30] 关振铎,张中太,焦金生.无机材料物理性能[M].2版.北京:清华大学出版社,2011.
GUAN Z D, ZHANG Z T, JIAO J S. Physical properties of inorganic materials[M]. 2nd ed. Beijing: Tsinghua University Press, 2011 (in Chinese).
[31] 段于森,张景贤,李晓光,等.稀土氧化物对常压烧结氮化硅陶瓷性能的影响[J].无机材料学报,2017,32(12):1275-1279.
DUAN Y S, ZHANG J X, LI X G, et al. Rare earth oxides on property of pressureless sintered Si₃N₄ ceramics[J]. Journal of Inorganic Materials, 2017, 32(12): 1275-1279 (in Chinese).
[32] 刘维良,刘绍洋,刘硕琦.自增韧Si₃N₄陶瓷的制备与性能研究[J].中国陶瓷,2011,47(11):12-14.
LIU W L, LIU S Y, LIU S Q. Study on the preparation and properties of self-toughened Si₃N₄ ceramics[J]. China Ceramics, 2011, 47(11): 12-14 (in Chinese).
[33] 魏赛,PORZ L W,谢志鹏,等.环境温度及晶界相断裂韧性对氮化硅陶瓷桥接行为的影响[J].稀有金属材料与工程,2015,44(s1):710-713.
WEI S, PORZ L W, XIE Z P, et al. Crack bridging in silicon nitride ceramics at various temperatures and grain boundary toughness[J]. Rare Metal Materials and Engineering, 2015, 44(s1): 710-713 (in Chinese).
[34] 王旭东,白彬.氮化硅陶瓷晶界相研究进展[J].材料导报,2016,30(s2):121-126.
WANG X D, BAI B. Research progress on grain boundary phase of silicon nitride ceramics[J]. Materials Review, 2016, 30(s2): 121-126 (in Chinese).
[35] LIU W, TONG W X, HE R X, et al. Effect of the Y₂O₃ additive concentration on the properties of a silicon nitride ceramic substrate[J]. Ceramics International, 2016, 42(16): 18641-18647.
[36] KITAYAMA M, HIRAO K, TORIYAMA M, et al. Thermal conductivity of β-Si₃N₄: I, effects of various microstructural factors[J]. Journal of the American Ceramic Society, 2004, 82(11): 3105-3112.
[37] YOKOTA H, ABE H, IBUKIYAMA M. Effect of lattice defects on the thermal conductivity of β-Si₃N₄[J]. Journal of the European Ceramic Society, 2003, 23(10): 1751-1759.
[38] WANG X L, XIE F W, ZHANG L Q, et al. Effect of vacancy defects on the thermal conductivity of graphene nanoribbons: a molecular dynamics study[J]. International Journal of Materials and Structural Integrity, 2012, 6(1): 26.
[39] WANG T, MADSEN G H, HARTMAIER A. Atomistic study of the influence of lattice defects on the thermal conductivity of silicon[J]. Modelling and Simulation in Materials Science and Engineering, 2014, 22(3): 035011.
[40] HU F, ZHU T B, XIE Z P, et al. Elimination of grain boundaries and its effect on the properties of silicon nitride ceramics[J]. Ceramics International, 2020, 46(8): 12606-12612.
[41] KIM J M, KO S I, KIM H N, et al. Effects of microstructure and intergranular glassy phases on thermal conductivity of silicon nitride[J]. Ceramics International, 2017, 43(7): 5441-5449.

Effect of Ternary Composite Sintering Agent Er₂O₃-Mg₂Si-Yb₂O₃ on Properties of Silicon Nitride Ceramics

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	ZHAN Lingli, HAN Lixiong, LI Jingwei, LI Hong, XIE Jun, XIONG Dehua. Structure and Performance of Glass-Ceramics with High Content of Coal Gangue Solid Waste [J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(4): 1124-1132.
[2]	GE Menglong, YE Qianqian, KANG Haijiao, LI Jianzhang. Research Progress of Admixture-Modified Magnesium Oxychloride Cement [J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(4): 1202-1210.
[3]	WEI Qi, LIU Yan, GENG Haining, MA Haosen, CHEN Wei, WANG Dongwen, PAN Sheqi, LI Qiu. Properties of Polyaluminum Sulfate-Modified Low-Alkalinity Cement [J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(4): 1237-1244.
[4]	CHEN Wei, SHENG Mingquan, XU Ao, LIANG Yue. Effects of High Temperature and Heating Rate on Gas Permeability and Porosity of Mortar [J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(4): 1256-1263.
[5]	ZHANG Chenming, HOU Dongshuai, ZHANG Hongzhi, ZHANG Wei. Peridynamic Simulation of Concrete Fracture Behavior under Uniaxial Tension [J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(4): 1276-1284.
[6]	LIU Guoqiang, LIU Laibao. Sulfate Corrosion Resistance of Concrete Mixed with Magnesia Expansive Agent [J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(4): 1293-1300.
[7]	WANG Tao, HOU Yunyi, MA Zhenfeng, YANG Xianlun, DUAN Yuxiu. Application of Fly Ash-Micro Silicon-Cement Ternary Composite Low Density Filling Cement Slurry in Shale Oil Horizontal Wells [J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(4): 1380-1387.
[8]	WANG Yuhua, SUN Shuanhu. Effect of Nano-SiO₂ on Early Properties and Microstructure of Fiber-Reinforced Ordinary Portland Cement-Sulphoaluminate Cement Composites [J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(3): 795-801.
[9]	XIAO Shuaipeng, LI Zongli, ZHANG Guohui, LI Changbing, LIU Shida, LI Yunbo. Effect of Thermal Fatigue on Mechanical Properties and Microstructure of Concrete [J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(3): 825-832.
[10]	ZHENG Li, CHEN Luyi, ZHANG Zhihao. Steel Fibre Parameter Optimization of Ultra-High Performance Concrete Based on Dense Particle Packing Theory [J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(3): 853-859.
[11]	AN Qiang, PAN Huimin, WANG Shuai, ZHAO Qingxin. Effects of Fly ash and Slag Particle Size Distributions on Microstructure and Chloride Ion Penetration Resistance of Concrete [J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(3): 884-893.
[12]	WANG Ruanbin, CHENG Liqian, LU Jingtong, JIN Ruoqi, HE Mingzhe, YAN Shuhao, JIANG Damei, DENG Shijie, CHU Xiangcheng. Preparation and Properties of Carbon Fiber Reinforced BT-HA Composites [J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(3): 994-1001.
[13]	CHEN Xin, CHEN Shikun, YAN Dongming, LIU Yi, WANG Tielong. Mechanical Properties of Magnesium Phosphate Coatings after High Temperature [J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(3): 1031-1038.
[14]	BAI Xiaotong, CUI Xiaorong, ZHANG Linrui, ZHOU Bingqing. Preparation of Sb₂Se₃ Film and Solar Cells with Different Substrate Inclination by VTD Method [J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(3): 1063-1068.
[15]	MU Changjiang, CHENG Kai, LIU Rui, JIA Enda, SUN Hao, NIU Teng, LU Xiaolei, DU Peng, YE Zhengmao. Cooperative Optimization of Mineral Admixtures of Cement-Based Grouting Materials for Semi-Flexible Pavement [J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(3): 1102-1112.