水基干压成型高导热氮化硅陶瓷的结构和性能
Structure and Properties of High Thermal Conductivity Silicon Nitride Ceramics by Aqueous Dry Pressing
摘 要
以α-Si3N4、β-Si3N4、MgO、Y2O3为原材料，利用以水为分散介质的水基干压成型工艺在不同温度（1 750，1 850℃）下烧结制备高导热氮化硅陶瓷，研究了不同烧结温度下陶瓷的结构、力学性能和热导率，并与以无水乙醇作为分散介质的非水基干压成型氮化硅陶瓷进行对比。结果表明：陶瓷的晶粒均呈长柱状，并且零散的粗大晶粒周围分布着较多的细长晶粒，呈双模式组织结构；1 750，1 850℃烧结温度下水基干压成型陶瓷的抗弯强度分别为555.7，747.5 MPa，断裂韧度分别为8.14，8.25 MPa·m1/2，均略低于非水基干压成型陶瓷，相对密度分别为99.00%，99.58%，平均晶粒尺寸分别为1.06，1.27 μm，热导率分别为65.70，75.54 W·m-1·K-1，均略高于非水基干压成型陶瓷。
分散介质
热导率
力学性能
silicon nitride ceramics
disperse medium
thermal conductivity
mechanical property
Abstract
High thermal conductivity silicon nitride ceramics were prepared by aqueous dry pressing process with water as dispersing medium and sintering at different temperatures (1 750, 1 850℃) using α-Si3N4, β-Si3N4, MgO, Y2O3 as raw materials. The structure, mechanical properties and thermal conductivity of the ceramics at different sintering temperatures were studied and compared with those of non-aqueous dry pressed silicon nitride ceramics with anhydrous ethanol as the dispersing medium. The results show that the grains of the ceramics were all long columnar, and there were many slender grains distributed around the scattered coarse grains, showing a dual-mode structure. At the sintering temperature of 1 750, 1 850℃, the bending strengths of aqueous dry pressed ceramics were 555.7, 747.5 MPa, and the fracture toughnesses were 8.14, 8.25 MPa·m1/2, respectively, which were slightly lower than those of non-aqueous dry pressed ceramics; the relative densities were 99.00%, 99.58%, the average grain sizes were 1.06,1.27 μm, and thermal conductivities were 65.70,75.54 W·m-1·K-1, respectively, which were slightly higher than those of non-aqueous dry pressed ceramics.
中图分类号 TQ127.2 DOI 10.11973/jxgccl202309008
所属栏目 材料性能及应用
基金项目
收稿日期 2022/5/11
修改稿日期 2023/5/29
网络出版日期
作者单位点击查看
备注田云龙(1995-),男,江苏无锡人,硕士研究生
引用该论文: TIAN Yunlong,QI Hai,ZHANG Peizhi,GUO Fangquan,HAN Weiyue. Structure and Properties of High Thermal Conductivity Silicon Nitride Ceramics by Aqueous Dry Pressing[J]. Materials for mechancial engineering, 2023, 47(9): 46～51
田云龙,祁海,张培志,郭方全,韩伟月. 水基干压成型高导热氮化硅陶瓷的结构和性能[J]. 机械工程材料, 2023, 47(9): 46～51
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参考文献
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【2】ZHOU Y, HYUGA H, KUSANO D, et al.A tough silicon nitride ceramic with high thermal conductivity[J].Advanced Materials, 2011, 23(39):4563-4567.
【3】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.
【4】梁振华, 彭桂花, 李庆余, 等.以MgSiN2作烧结助剂制备高热导β-Si3N4陶瓷[J].硅酸盐学报, 2010, 38(10):1948-1952. LIANG Z H, PENG G H, LI Q Y, et al.Fabrication of high thermal conductivity β-Si3N4 ceramics with MgSiN2 as additive[J].Journal of the Chinese Ceramic Society, 2010, 38(10):1948-1952.
【5】DUAN Y S, ZHANG J X, LI X G, et al.High thermal conductivity silicon nitride ceramics prepared by pressureless sintering with ternary sintering additives[J].International Journal of Applied Ceramic Technology, 2019, 16(4):1399-1406.
【6】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.
【7】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.
【8】KITAYAMA M, HIRAO K, TSUGE A, et al.Thermal conductivity of β-Si3N4:II, effect of lattice oxygen[J].Journal of the American Ceramic Society, 2004, 83(8):1985-1992.
【9】黄勇, 向军辉, 谢志鹏, 等.陶瓷材料流延成型研究现状[J].硅酸盐通报, 2001, 20(5):22-27. HUANG Y, XIANG J H, XIE Z P, et al.Present status of research on tape-casting technology for ceramic materials[J].Bulletin of the Chinese Ceramic Society, 2001, 20(5):22-27.
【10】YANG C P, LIU Q A, ZHANG B A, et al.Effect of MgF2 addition on mechanical properties and thermal conductivity of silicon nitride ceramics[J].Ceramics International, 2019, 45(10):12757-12763.
【11】梁振华, 彭桂花, 李庆余, 等.以MgSiN2作烧结助剂制备高热导β-Si3N4陶瓷[J].硅酸盐学报, 2010, 38(10):1948-1952. LIANG Z H, PENG G H, LI Q Y, et al.Fabrication of high thermal conductivity β-Si3N4 ceramics with mgsin2 as additive[J].Journal of the Chinese Ceramic Society, 2010, 38(10):1948-1952.
【12】王月民, 刘军, 王超, 等.压力对凝胶注模成型95氧化铝陶瓷性能的影响[J].硅酸盐通报, 2012, 31(5):1223-1227. WANG Y M, LIU J, WANG C, et al.Influence of pressure on properties of 95 alumina ceramics prepared by gelcasting forming[J].Bulletin of the Chinese Ceramic Society, 2012, 31(5):1223-1227.
【13】左春阳.粉体压制工艺过程机理及优化控制研究[D].广州:华南理工大学, 2019. ZUO C Y.Research on mechanism and optimization control of powder pressing process[D].Guangzhou:South China University of Technology, 2019.
【14】杜苗凤, 张培志, 郭方全, 等.粉料和冷等静压对凝胶注模成型Al2O3陶瓷致密化的影响[J].机械工程材料, 2020, 44(10):28-32. DU M F, ZHANG P Z, GUO F Q, et al.Effect of powder and cold isostatic pressing on densification of Al2O3 ceramics molded by gelcasting[J].Materials for Mechanical Engineering, 2020, 44(10):28-32.
【15】KULIG M, GREIL P.Surface chemistry and suspension stability of oxide-nitride powder mixtures[J].Journal of Materials Science, 1991, 26(1):216-224.
【16】MITOMO M.Pressure sintering of Si3N4[J].Journal of Materials Science, 1976, 11(6):1103-1107.
【17】林森.高热导氮化硅陶瓷制备及性能研究[D].北京:中国科学院大学, 2013. LIN S.Preparation and properties of silicon nitride ceramics with high thermal conductivity[D].Beijing:University of Chinese Academy of Sciences, 2013.
【18】张晶, 王文雪, 孙峰, 等.烧结温度对氮化硅陶瓷球显微结构和力学性能的影响[J].硅酸盐通报, 2021, 40(1):252-257. ZHANG J, WANG W X, SUN F, et al.Effect of sintering temperature on microstructure and mechanical properties of silicon nitride ceramic balls[J].Bulletin of the Chinese Ceramic Society, 2021, 40(1):252-257.
【19】张洁, 宁晓山, 吕鑫, 等.含稀土助烧剂氮化硅陶瓷的热导率、强度及电学性能[J].稀有金属材料与工程, 2008, 37(增刊1):693-696. ZHANG J, NING X S, LYU X, et al.Effect of rare-earth additives on thermal conductivity, mechanical and electrical properties of silicon nitride ceramics[J].Rare Metal Materials and Engineering, 2008, 37(S1):693-696.
【20】HIROSAKI N, OKAMOTO Y, MUNAKATA F, et al.Effect of seeding on the thermal conductivity of self-reinforced silicon nitride[J].Journal of the European Ceramic Society, 1999, 19(12):2183-2187.
【21】YOKOTA H, IBUKIYAMA M.Effect of lattice impurities on the thermal conductivity of β-Si3N4[J].Journal of the European Ceramic Society, 2003, 23(1):55-60.
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