熔盐辅助合成Dy3Si2C2包裹SiC粉体及其陶瓷的烧结行为

doi:10.15541/jim20200068

无机材料学报 ›› 2021, Vol. 36 ›› Issue (1): 49-54.DOI: 10.15541/jim20200068 CSTR: 32189.14.10.15541/jim20200068

所属专题：副主编黄庆研究员专辑；优秀作者论文集锦

熔盐辅助合成Dy₃Si₂C₂包裹SiC粉体及其陶瓷的烧结行为

万朋^1,²,李勉¹,黄庆¹()

^1. 中国科学院宁波材料技术与工程研究所先进能源材料工程实验室(筹), 宁波 315201
^2. 西安交通大学金属材料强度国家重点实验室, 西安 710049

收稿日期:2020-02-15 修回日期:2020-07-15 出版日期:2021-01-20 网络出版日期:2020-08-28
作者简介:万朋(1993-), 男, 硕士研究生. E-mail: wanpeng@nimte.ac.cn
基金资助:
国家自然科学基金(21671195);国家自然科学基金(51902320)

Molten Salt Assisted Synthesis of Dy₃Si₂C₂ Coated SiC Powders and Sintering Behavior of SiC Ceramics

WAN Peng^1,²,LI Mian¹,HUANG Qing¹()

^1. Engineering Laboratory of Advanced Energy Materials, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, China
^2. State Key Laboratory for Mechanical Behavior of Materials, Xi’an Jiaotong University, Xi’an 710049, China;

Received:2020-02-15 Revised:2020-07-15 Published:2021-01-20 Online:2020-08-28
About author:WAN Peng(1993-), male, Master candidate. E-mail: wanpeng@nimte.ac.cn
Supported by:
National Natural Science Foundation of China(21671195);National Natural Science Foundation of China(51902320)

摘要/Abstract

摘要：

碳化硅陶瓷因自身优良的物理化学性能而具有广泛的应用前景。碳化硅的化学键结合特性决定了其难以烧结成型, 因此如何制备高质量碳化硅陶瓷是领域内的难点之一。本研究以三元稀土碳化物Dy₃Si₂C₂作为新型SiC陶瓷的烧结助剂, 依据Dy-Si-C体系的高温相转变原位促进碳化硅的烧结致密化。采用放电等离子烧结技术, 利用金属Dy与SiC反应生成Dy₃Si₂C₂, 对Dy₃Si₂C₂包裹的SiC粉体进行烧结。在1800 ℃、45 MPa的烧结条件下, 得到了致密度为99%、热导率为162.8 W·m ^-1·K ^-1的高纯度碳化硅陶瓷。进一步的研究表明, 高温下Dy₃Si₂C₂与SiC发生共晶反应, 在晶界处产生的液相促进了SiC陶瓷的致密化, 表明稀土层状碳化物Re₃Si₂C₂(Re=La, Ce…)有助于SiC的烧结致密。

关键词: SiC, Dy₃Si₂C₂, 放电等离子烧结, 熔盐

Abstract:

Silicon carbide is widely used because of its excellent physical and chemical properties. The chemical bonding characteristics of SiC make it difficult to be sintered. Therefore, preparation of high-quality SiC ceramics is one of the challenges in SiC research field. In this study, the ternary rare-earth carbide Dy₃Si₂C₂ was proposed as a new sintering additive for SiC ceramics, through the phase transition of Dy-Si-C system at high temperatures to promote the densification of SiC. The Dy₃Si₂C₂ coated SiC powders were synthesized via an in-situ reaction between metal Dy and SiC in high temperature molten salts. The Dy₃Si₂C₂ coated SiC powder was sintered by spark plasma sintering (SPS), at 1800 ℃, 45 MPa. As the result, high-purity SiC ceramic with the density of 99% and thermal conductivity of 162.8 W·m ^-1·K ^-1was obtained to form the SiC-Dy₃Si₂C₂raw material with n(Dy) : n(SiC)=1 : 4. Further study shows that Dy₃Si₂C₂ and SiC undergo a eutectic reaction at high temperatures, which generates liquid phase at the grain boundaries and promotes the densification of SiC ceramics. This study shows that the ternary rare-earth carbides Re₃Si₂C₂ (Re=La, Ce…) has great potential to be used as the sintering additive for SiC.

Key words: SiC, Dy₃Si₂C₂, spark plasma sintering, molten salt

中图分类号:

TQ174

万朋, 李勉, 黄庆. 熔盐辅助合成Dy₃Si₂C₂包裹SiC粉体及其陶瓷的烧结行为[J]. 无机材料学报, 2021, 36(1): 49-54.

WAN Peng, LI Mian, HUANG Qing. Molten Salt Assisted Synthesis of Dy₃Si₂C₂ Coated SiC Powders and Sintering Behavior of SiC Ceramics[J]. Journal of Inorganic Materials, 2021, 36(1): 49-54.

图/表 5

图1 (a) SiC粉与不同配比制备的SiC-Dy3Si2C2复合粉体的XRD图谱, (b) SiC原始粉体和(c) SiC-Dy3Si2C2复合粉体的SEM照片

Fig. 1 (a) XRD patterns of the SiC and SiC-Dy3Si2C2 raw materials prepared with different molar ratios, SEM images of (b) SiC and (c) SiC-Dy3Si2C2

图2 不同配比和在不同温度烧结SiC陶瓷的(a)XRD图谱及(b~f)SEM照片

Fig. 2 (a) XRD and (b-f) SEM images of sintered pure SiC ceramics and SiC ceramics sintered from SiC-Dy3Si2C2 raw materials with different molar ratios (b) SiC; (c) n(Dy) : n(SiC) =1 : 8, 1800 ℃; (d) n(Dy) : n(SiC) =1 : 6, 1800℃; (e) n(Dy) : n(SiC)=1 : 4, 1800 ℃; (f) n(Dy) : n(SiC)=1 : 4, 1700 ℃

图3 用n(Dy) : n(SiC)=1 : 4的粉体烧结成SiC陶瓷的(a)TEM照片、(b)能谱图像、(c)图(a)中标记1处和(d) 2处的高分辨HR-TEM照片

Fig. 3 (a) TEM image and (b) EDS analysis of SiC ceramics sintered from raw materials with ratio of n(Dy) : n(SiC)=1 : 4; (c) HR-TEM of the marked area 1 in (a); (d) HR-TEM image of the marked area 2 in (a)

图4 用SPS烧结SiC陶瓷的压头位移曲线

Fig. 4 Displacement curves of piston on the SiC ceramic during the SPS sintering

表1 SiC陶瓷的密度和热物理参数

Table 1 Parameters of density and thermal properties of sintered SiC ceramics

Specimen	Density /(g·cm^-3)	Heat capacity /(J·g^-1·K^-1)	Thermal diffusion /(mm²·s^-1)	Phonon mean free path/nm	Thermal conductivity /(W·m^-1·K^-1)
n(Dy) : n(SiC)=1 : 8(1800 ℃)	3.321	0.649	54.3	13.8	117.1
n(Dy) : n(SiC)=1 : 6(1800 ℃)	3.589	0.533	52.1	13.2	99.8
n(Dy) : n(SiC)=1 : 4(1800 ℃)	3.228	0.683	73.8	18.7	162.8
n(Dy) : n(SiC)=1 : 4(1700 ℃)	3.306	0.648	58.0	16.5	124.3

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熔盐辅助合成Dy₃Si₂C₂包裹SiC粉体及其陶瓷的烧结行为

Molten Salt Assisted Synthesis of Dy₃Si₂C₂ Coated SiC Powders and Sintering Behavior of SiC Ceramics

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