基于Si3N4@MgSiN2核壳结构粉体制备&#x003b2;-Si3N4晶须

王为得; 刘一铭; 潘勇; 莫勇; 王伟明; 马青松

doi:10.19976/j.cnki.43-1448/TF.2024078

粉末冶金材料科学与工程 >

2025 , Vol. 30 >Issue 1: 1 - 10

DOI: https://doi.org/10.19976/j.cnki.43-1448/TF.2024078

工艺技术

基于Si₃N₄@MgSiN₂核壳结构粉体制备β-Si₃N₄晶须

王为得 ,
刘一铭 ,
潘勇 ,
莫勇 ,
王伟明 ,
马青松

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1.国防科技大学前沿交叉学科学院,长沙 410073;
2.国防科技大学空天科学学院新型陶瓷纤维及其复合材料重点实验室,长沙 410073;
3.中国运载火箭技术研究院空间物理重点实验室,北京 100076

收稿日期: 2024-09-20

修回日期: 2025-01-02

网络出版日期: 2025-04-08

基金资助

国家自然科学基金资助项目(52202077); 国防科技重点实验室基金资助项目(6142907220303); 国防科技基础加强计划资助项目(2022-JCJQ-LB-073); 湖南省自然科学基金资助项目(2024JJ5407)

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β-Si₃N₄ whiskers preparation from Si₃N₄@MgSiN₂ core-shell structure powders

WANG Weide ,
LIU Yiming ,
PAN Yong ,
MO Yong ,
WANG Weiming ,
MA Qingsong

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1. College of Advanced Interdisciplinary Studies, National University of Defense Technology, Changsha 410073, China;
2. Science and Technology on Advanced Ceramic Fibers and Composites Laboratory, College of Aerospace Science and Engineering, National University of Defense Technology, Changsha 410073, China;
3. Science and Technology on Space Physics Labrotary, China Academy of Launch Vehicle Technology,Beijing 100076, China

Received date: 2024-09-20

Revised date: 2025-01-02

Online published: 2025-04-08

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摘要

一维单晶β-Si₃N₄晶须兼具优异的热学、力学、耐高温、耐腐蚀等性能,广泛用作树脂基、金属基及陶瓷基的增强体材料。以氧化物为烧结助剂制备的β-Si₃N₄晶须存在残留杂质多、长径比低等不足,限制了其增强效果。本研究借助熔盐法在较低温度下制备壳层厚度可控的Si₃N₄@MgSiN₂核壳结构粉体,再以此粉体为原料烧结制备β-Si₃N₄晶须,采用X射线衍射仪、能谱仪和扫描电子显微镜研究粉体和晶须的物相组成和微观形貌。结果表明：在高温下,α-Si₃N₄在壳层MgSiN₂形成的液相中通过“溶解析出”机制实现相转变和Ostwald熟化,形成了高长径比的β-Si₃N₄晶须。升高烧结温度及提高原料中Mg/Si₃N₄质量比均可增强液相中的扩散传质,有利于晶须沿[001]方向生长,表现为晶须的长度和长径比增大。同时,MgSiN₂在高温下不稳定的特性促使其分解为Mg、N₂及Si₃N₄,保证了晶须的高纯度。因此,在1 750 ℃烧结1 h可制备高纯度、高长径比、易分散的β-Si₃N₄晶须。本研究提出的晶须新型制备策略经济可行,为高性能β-Si₃N₄晶须的制备提供了新途径。

关键词： β-Si₃N₄晶须; 熔盐法; 烧结助剂; 核壳结构; 生长机制

本文引用格式

王为得 , 刘一铭 , 潘勇 , 莫勇 , 王伟明 , 马青松 . 基于Si₃N₄@MgSiN₂核壳结构粉体制备β-Si₃N₄晶须[J]. 粉末冶金材料科学与工程, 2025 , 30(1) : 1 -10 . DOI: 10.19976/j.cnki.43-1448/TF.2024078

Abstract

One dimensional single crystal β-Si₃N₄ whiskers possess excellent thermal, mechanical, high- temperature and corrosion resistance properties, and are widely used as resin based, metal based, and ceramic based reinforcement materials. β-Si₃N₄ whiskers prepared with oxides as sintering aids have shortcomings such as high residual impurities and low aspect ratio, which limit their reinforcement effect. This study utilized the molten salt synthesis to prepare Si₃N₄@MgSiN₂ core-shell structured powders with controllable shell thickness at lower temperature, and further prepared β-Si₃N₄ whiskers from this powder through sintering. The phase composition and microstructure of powders and whiskers were studied using X-ray diffractometer, energy dispersive spectrometer, and scanning electron microscope. The results show that at high temperatures, α-Si₃N₄ undergoes a phase transformation and Ostwald ripening in the liquid phase formed by the shell MgSiN₂ through a “dissolution-precipitation” mechanism, resulting in the formation of β-Si₃N₄ whiskers with high aspect ratio. Raising the sintering temperature and increasing the Mg/Si₃N₄ mass ratio in the raw material can enhance the diffusion mass transfer in the liquid phase, which is beneficial for the growth of whiskers along the [001] direction, manifest as an increase in whisker length and aspect ratio. At the same time, the unstable nature of MgSiN₂ at high temperature promotes its decomposition into Mg, N₂, and Si₃N₄, ensuring the high purity of the whiskers. Therefore, high-purity, high aspect ratio, and easily dispersible β-Si₃N₄ whiskers are prepared by sintering at 1 750 ℃ for 1 h. The new preparation strategy of whiskers proposed in this study is economically feasible and provides a new approach for the preparation of high-performance β-Si₃N₄ whiskers.

Key words： β-Si₃N₄ whisker; molten salt synthesis; sintering aid; core-shell structure; growth mechanism

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