低温反应熔渗工艺制备AlN-SiC复相陶瓷及其性能研究

doi:10.15541/jim20230091

无机材料学报 ›› 2023, Vol. 38 ›› Issue (10): 1223-1229.DOI: 10.15541/jim20230091 CSTR: 32189.14.10.15541/jim20230091

所属专题：【结构材料】高导热陶瓷(202409)；【结构材料】陶瓷基复合材料(202409)

低温反应熔渗工艺制备AlN-SiC复相陶瓷及其性能研究

孙小凡¹^,²(), 陈小武¹^,², 靳喜海¹^,²(), 阚艳梅¹^,², 胡建宝¹^,², 董绍明¹^,²()

1.中国科学院上海硅酸盐研究所高性能陶瓷和超微结构国家重点实验室, 上海 200050
2.中国科学院大学材料与光电研究中心, 北京 100049

收稿日期:2023-02-22 修回日期:2023-04-20 出版日期:2023-10-20 网络出版日期:2023-05-15
通讯作者: 靳喜海, 研究员. E-mail: jinxihai@hotmail.com;
董绍明, 研究员. E-mail: smdong@mail.sic.ac.cn
作者简介:孙小凡(1998-), 男, 硕士研究生. E-mail: 2487801767@qq.com

Fabrication and Properties of AlN-SiC Multiphase Ceramics via Low Temperature Reactive Melt Infiltration

SUN Xiaofan¹^,²(), CHEN Xiaowu¹^,², JIN Xihai¹^,²(), KAN Yanmei¹^,², HU Jianbao¹^,², DONG Shaoming¹^,²()

1. State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China
2. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

Received:2023-02-22 Revised:2023-04-20 Published:2023-10-20 Online:2023-05-15
Contact: JIN Xihai, professor. E-mail: jinxihai@hotmail.com;
DONG Shaoming, professor. E-mail: smdong@mail.sic.ac.cn
About author:SUN Xiaofan (1998-), male, Master candidate. E-mail: 2487801767@qq.com
Supported by:
National Natural Science Foundation of China(52172111);National Natural Science Foundation of China(51872310);National Key R&D Program of China(2022YFB3707700)

摘要/Abstract

摘要：

AlN-SiC复相陶瓷力学性能好、导热性与抗高温氧化性能优异, 作为纤维增强陶瓷基复合材料的基体材料具有良好的应用前景。本研究以Si-Al合金为熔渗介质, 多孔C-Si₃N₄为熔渗预制体, 对低温反应熔渗制备AlN-SiC复相陶瓷及其性能展开研究。研究发现Si-Al合金形态对反应熔渗过程存在着重要的影响: 以Si-Al合金粉末作为熔渗介质时, 反应熔渗过程中在Si-Al/C-Si₃N₄界面处将原位形成一层致密的Al-O阻挡层, 从而严重阻碍Si-Al熔体向C-Si₃N₄预制体内部的渗透, 使反应熔渗过程难以进行；以Si-Al合金锭作为熔渗介质时, Si-Al熔体可以深入渗透到多孔C-Si₃N₄预制体内部, 并通过进一步反应, 原位形成致密的AlN-SiC复相陶瓷。材料性能测试表明, 所得材料的力学和热学性能与其内部残余硅含量关系密切。随着残余硅含量降低, 材料强度明显提升, 而热导率有所下降。含质量分数4%残余硅的AlN-SiC复相陶瓷, 抗弯强度达到320.1 MPa, 热导率达26.3 W·m^-1·K^-1, 材料的强度几乎与传统反应烧结SiC陶瓷相当, 并深入探讨了出现上述现象的本质原因。本研究对低温熔渗工艺制备SiC_f/AlN-SiC复合材料具有重要的指导意义。

关键词: 反应熔渗(RMI), AlN-SiC, 机械性能, 热导率

Abstract:

AlN-SiC multiphase ceramics possess robust mechanical strength, high thermal conductivity and good oxidization resistance, and show great potential as the matrix material of fiber reinforced ceramic matrix composites. In this work, AlN-SiC multiphase ceramics were fabricated via low temperature reactive melt infiltration of Si-Al alloy into porous C-Si₃N₄ preforms. Influence of Si-Al source on the melt infiltration process was studied, and impact of residual silicon on the mechanical and thermal properties of the AlN-SiC ceramics was investigated. It was found that an Al-O layer was in-situ formed at the interface between Si-Al melt and C-Si₃N₄ preform, when Si-Al powder was used as the infiltration medium. This seriously retarded the melt infiltration process and made the penetration of Si-Al melt into the C-Si₃N₄ preform hardly possible. However, when Si-Al ingot was used as the infiltration medium, a well infiltration of Si-Al melt into the C-Si₃N₄ preform occurred, which led to the formation of dense AlN-SiC ceramics. Mechanical and thermal property measurements indicated that the strength of the AlN-SiC ceramics was significantly improved as the residual silicon content in it was reduced, while a reverse trend was observed for the thermal conductivity. AlN-SiC ceramics with 4%(in mass) residual silicon showed a high strength of 320.1 MPa, nearly comparable to that of conventional reaction bonded SiC, although its thermal conductivity was modest (26.3 W·m^-1·K^-1). The fundamental reasons for the above phenomena were discussed. This study is of great significance for the preparation of SiC_f/AlN-SiC composites by low temperature reactive melt infiltration.

Key words: reactive melt infiltration (RMI), AlN-SiC, mechanical property, thermal conductivity

中图分类号:

TB484

孙小凡, 陈小武, 靳喜海, 阚艳梅, 胡建宝, 董绍明. 低温反应熔渗工艺制备AlN-SiC复相陶瓷及其性能研究[J]. 无机材料学报, 2023, 38(10): 1223-1229.

SUN Xiaofan, CHEN Xiaowu, JIN Xihai, KAN Yanmei, HU Jianbao, DONG Shaoming. Fabrication and Properties of AlN-SiC Multiphase Ceramics via Low Temperature Reactive Melt Infiltration[J]. Journal of Inorganic Materials, 2023, 38(10): 1223-1229.

图/表 8

Table 1 Chemical composition of the slurries used for different types of C-Si3N4 infiltration preform preparation

Material	Mass percent of LCP/%	Mass percent of HCP/%
α-Si₃N₄	20.17	15.66
Carbon black	8.65	6.71
Phenolic resin	17.29	26.85
Dibutyl phthalate (DBP)	5.76	4.47
Polyvinyl butyral (PVB)	7.20	5.59
Castor oil	0.58	0.45
Ethanol absolute	40.35	40.27

Fig. 1 SEM images of porous C-Si3N4 infiltration preforms with different carbon contents (a, b) Low carbon content preform (LCP); (c, d) High carbon content preform (HCP)

Fig. 2 Mercury porosimetry curves of the C-Si3N4 infiltration preforms with different carbon contents (a) Cumulative volume percentage vs pore diameter; (b) Incremental intrusion vs pore diameter

Fig. 3 SEM image and EDS line scanning of the melt/preform interface region in the post melt infiltrated Si-Al/C-Si3N4 system, using (a, b) Si-Al ingot and (c, d) Si-Al powder as infiltration medium Colorful figures are available on the website

Fig. 4 (a) XRD patterns of AlN-SiC multiphase ceramics prepared from different types of C-Si3N4 preform, and (b) changes of standard Gibbs free energy of reaction (3-6) as a function of temperatures calculated with HSC 6.0 software

Fig. 5 SEM images of AlN-SiC multiphase ceramics prepared from different C-Si3N4 preforms and their corresponding EDS mapping (a-e) Low carbon content preform; (f-j) High carbon content preform

Table 2 Density and mechanical properties of AlN-SiC multiphase ceramics prepared from different types of C-Si3N4 preform

Preform type	Bulk density/ (g·cm^-3)	Hardness/GPa	Bending strength/MPa
LCP	2.83	12.8±0.2	198.3±4.6
HCP	2.95	16.9±0.4	320.1±25.1

Fig. 6 Thermal diffusivity (a), specific heat (b) and thermal conductivity (c) of AlN-SiC ceramics prepared from the LCP and HCP preforms

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低温反应熔渗工艺制备AlN-SiC复相陶瓷及其性能研究

Fabrication and Properties of AlN-SiC Multiphase Ceramics via Low Temperature Reactive Melt Infiltration

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