以AC发泡剂为添加剂燃烧合成α-Si3N4粉体

doi:10.3724/SP.J.1077.2012.00169

无机材料学报 ›› 2012, Vol. 27 ›› Issue (2): 169-173.DOI: 10.3724/SP.J.1077.2012.00169 CSTR: 32189.14.SP.J.1077.2012.00169

以AC发泡剂为添加剂燃烧合成α-Si₃N₄粉体

陈义祥¹, 杨建辉^1,2, 蒋志君³, 林志明¹, 李江涛¹

(1. 中国科学院理化技术研究所, 北京 100190; 2. 中国科学院研究生院, 北京 100039; 3. 科技部高技术研究发展中心, 北京 100044)

收稿日期:2011-02-14 修回日期:2011-03-28 出版日期:2012-02-10 网络出版日期:2012-01-05
作者简介:陈义祥(1980-), 男, 博士, 助理研究员. E-mail: yxchen@mail.ipc.ac.cn
基金资助:
国家自然科学基金(50772116, 50932006) National Natural Science Foundation of China (50772116, 50932006)

Combustion Synthesis of α-Si₃N₄ Powder Using AC as Additive

CHEN Yi-Xiang¹, YANG Jian-Hui^1,2, JIANG Zhi-Jun³, LIN Zhi-Ming¹, LI Jiang-Tao¹

(1. Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, China; 2. Graduate School of the Chinese Academy of Science, Beijing 100039, China; 3. High-Technology R&D Center, The Ministry of Science and Technology of the People′s Republic of China, Beijing 100044, China)

Received:2011-02-14 Revised:2011-03-28 Published:2012-02-10 Online:2012-01-05
About author:CHEN Yi-Xiang. E-mail: yxchen@mail.ipc.ac.cn

摘要/Abstract

摘要：

以硅粉和Si₃N₄粉体为反应剂, 偶氮二甲酰胺(AC发泡剂)为添加剂, 利用燃烧合成技术在较低氮气压力下制备了高α相含量的Si₃N₄粉体. 采用X射线衍射和扫描电镜分别对产物的物相组成及显微结构进行了表征, 研究了AC发泡剂对α相Si₃N₄粉体的形成和产物颗粒形貌的影响. 结果表明, AC发泡剂能促进硅粉快速氮化, 产物中α-Si₃N₄的含量随着AC发泡剂添加量的增加而增加. 当AC发泡剂的添加量为24wt%时, 产物中α-Si₃N₄的含量高达85.2wt%. 对AC发泡剂作用下的燃烧合成Si₃N₄的反应机理做了初步探讨, 研究表明: AC发泡剂的分解产物N₂、CO、NH₃不仅增加了坯体的透气性, 而且改变了燃烧反应的传热和传质路线, 从而促进了硅粉快速氮化和α-Si₃N₄粉体的生成.

关键词: AC发泡剂, Si₃N₄, 燃烧合成

Abstract:

Combustion synthesis (CS) of high content of α-Si₃N₄ powders was carried out using Si and Si₃N₄ powders as reactants with the addition of diazenedicarboxamide (AC) at a relatively low N₂ pressure of 3 MPa. The phase compositions and microstructure of products were characterized by XRD and SEM. Effects of AC contents on the phase compositions and Si₃N₄ particles morphology were studied. In addition, the reaction mechanisms were discussed. The results indicated that the additive AC promoted the nitridation of Si. The α-Si₃N₄ contents in the combustion-synthesized products showed great dependence on the contents of AC added in the reactants, which reached 85.2wt% adding with 24wt% AC. Meanwhile, impurities such as SiC, Si₂N₂O could be found in the final products when more than 12wt% AC agent was added. Poor dispersibility of Si₃N₄ particles would be more serious with increasing AC contents in the reactants. N₂, CO and NH₃ produced by decomposition of AC leaded to a change of compact porosity, thermal convection and mass transfer processes, which was responsible for the increasing contents of α-Si₃N₄ and the discrepancy morphology of the products.

Key words: AC foaming agent, Si₃N₄, combustion synthesis

中图分类号:

TG164

陈义祥, 杨建辉, 蒋志君, 林志明, 李江涛. 以AC发泡剂为添加剂燃烧合成α-Si₃N₄粉体[J]. 无机材料学报, 2012, 27(2): 169-173.

CHEN Yi-Xiang, YANG Jian-Hui, JIANG Zhi-Jun, LIN Zhi-Ming, LI Jiang-Tao. Combustion Synthesis of α-Si₃N₄ Powder Using AC as Additive[J]. Journal of Inorganic Materials, 2012, 27(2): 169-173.

图/表 3

图1 样品A0-A6燃烧合成产物的XRD图谱

Fig. 1 XRD patterns of the combustion products from A0-A6

图2 燃烧产物中α-Si3N4含量随AC添加量的变化曲线

Fig. 2 Variation of α-Si3N4 contents in the combustion products with different percentages of AC

图3 AC发泡剂添加量不同时对应的燃烧合成产物的SEM照片

Fig. 3 SEM images of combustion products synthesized using different percentages of AC in starting materials

参考文献 15

[1]	Shibata N, Pennycook S, Gosnell T, et al. Observation of rare-earth segregation in silicon nitride ceramics at subnanometre dimensions. Nature, 2004, 428: 730-733.
[2]	LUO Min, CHENG Jia, MA Jing, et al. Biomimetic synthesis of porous Si3N4 ceramics. Journal of Inorganic Materials, 2008, 23(4): 763-768.
[3]	WANG Yong, WO Yin-Hua, YAO Kui-Hong, et al. CVD Synthesis of silicon nitride (SiN) nanopowders in a novel two-stage fluidized bed reactor. Journal of Inorganic Materials, 2006, 21(1): 41-45.
[4]	LIU Xue-Jian, HUANG Zhi-Yong, HUANG Li-Ping, et al. Mechanical properties and microstructure of silicon nitride ceramics by pressureless sintering. Journal of Inorganic Materials, 2004, 19(6): 1282-1286.
[5]	Riley F L. Silicon nitride and related materials. J. Am. Ceram. Soc., 2000, 83(2): 245-265.
[6]	Zakorzhevskii V V, Borovinskaya I P. Some regularities of synthesis α-Si3N4 in a commercial SHS reactor. International Journal of Self-Propagating High-Temperature Synthesis, 2000, 19(2): 171-191.
[7]	陈义祥, 林志明, 李江涛, 等(CHEN Yi-Xiang, et al). PTFE添加剂对燃烧合成氮化硅的影响. 稀有金属材料与工程(Rare Metal Mat. Eng.), 2007, 36(3): 661-664.
[8]	Yang Y, Chen Y X, Lin Z M, et al. Synthesis of α-Si3N4 using low-α-phase Si3N4 diluent by the seeding technique. Scripta Materialia, 2007, 56: 401-404.
[9]	Jin H B, Yang Y, Chen Y X, et al. Mechanochemical-activation -assisted combustion synthesis of α-Si3N4. J. Am. Ceram. Soc., 2006, 89(3): 1099-1102.
[10]	Cao Y G, Chen H, Li J T, et al. Formation of α-Si3N4 whiskers with addition of NaN3 as catalyst. Journal of Crystal Growth, 2002, 234(1): 9-11.
[11]	Jiang J X. A new synthesis method of α-silicon nitride powder reductive combustion synthesis from silicon and silicon dioxide. J. Am. Ceram. Soc., 2009, 92(12): 3095-3097.
[12]	Gazzara C P, Messier D R. Determination of phase content of Si3N4 by X-ray diffraction analysis. Am. Ceram. Bull., 1977, 56(9): 777-780.
[13]	刘建国, 龚元姞. 偶氮二甲酞胺发泡剂综述. 原材料, 2000(2): 17-20.
[14]	Lange H, Wötting G, Winter G. Silicon nitride from powder synthesis to ceramic material. Angew. Chem. Int. Ed. Engl., 1991, 30(12): 1579-1597.
[15]	Barinova T V, Borovinskaya I P. Combustion of silicon powders containing organic additives in nitrogen gas under pressure: 1. Effect of dopants on combustion phenomenology. International Journal of Self-Propagating High-Temperature Synthesis, 2009, 18(1): 25-29.

以AC发泡剂为添加剂燃烧合成α-Si₃N₄粉体

Combustion Synthesis of α-Si₃N₄ Powder Using AC as Additive

RichHTML

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

图/表 3

参考文献 15

相关文章 15

编辑推荐

Metrics

本文评价

[1]	邱子豪, 田志林, 郑丽雅, 李斌. Si₃N₄陶瓷在高温熔盐-水氧环境下的腐蚀行为[J]. 无机材料学报, 2024, 39(3): 274-282.
[2]	苏浩健, 周敏, 李来风. 多元素掺杂优化SnTe的热电性能[J]. 无机材料学报, 2024, 39(10): 1159-1166.
[3]	张叶, 姚冬旭, 左开慧, 夏咏锋, 尹金伟, 曾宇平. 原位引入BN-SiC燃烧合成Si₃N₄-BN-SiC复合材料[J]. 无机材料学报, 2022, 37(5): 574-578.
[4]	孟晴, 李江涛. 燃烧合成疏水BN粉体和超疏水涂层的制备及其性能表征[J]. 无机材料学报, 2022, 37(10): 1037-1042.
[5]	周鑫, 马垒, 刘涛, 郭永斌, 王岛, 董培林. Si₃N₄/FePd/Si₃N₄薄膜的晶体结构和磁性能研究[J]. 无机材料学报, 2018, 33(8): 909-913.
[6]	鱼银虎, 汪涛, 张洪敏, 张度宝, 潘剑锋. PTFE促发TiC陶瓷粉体低温固相合成研究[J]. 无机材料学报, 2015, 30(3): 272-276.
[7]	王贺云, 刘茜, 周遥, 周真真，刘光辉. 碳纤维复合Si₃N₄陶瓷材料的制备及性能研究[J]. 无机材料学报, 2014, 29(9): 1003-1008.
[8]	豆志河, 张廷安, 文明, 史冠勇, 赫冀成. 燃烧合成法制备NdB₆超细粉体及反应机理[J]. 无机材料学报, 2014, 29(7): 711-716.
[9]	胡海龙, 姚冬旭, 夏咏锋, 左开慧, 曾宇平. 反应烧结制备Si₃N₄/SiC复相陶瓷及其力学性能研究[J]. 无机材料学报, 2014, 29(6): 594-598.
[10]	喇培清, 韩少博, 卢学峰, 魏玉鹏. 稀释剂添加量对燃烧合成亚微米ZrB₂微观组织的影响[J]. 无机材料学报, 2014, 29(2): 191-196.
[11]	张英伟, 余建波, 夏咏锋, 左开慧, 姚冬旭, 曾宇平, 任忠鸣. 籽晶添加对氮化硅陶瓷显微结构与力学性能的影响[J]. 无机材料学报, 2012, 27(8): 807-812.
[12]	邹小庆, 周国红, 易海兰, 杨燕, 王士维. 燃烧法合成铪酸钇粉体及其透明陶瓷的制备[J]. 无机材料学报, 2011, 26(9): 929-932.
[13]	曾一明, 郑燕青,忻隽,孔海宽, 陈辉, 涂小牛,施尔畏. Si₃N₄ 晶体的压电性能第一性原理研究[J]. 无机材料学报, 2011, 26(2): 180-184.
[14]	陈刚,翟鹏程,张清杰. Si₃N₄陶瓷蠕变性能MSP评价方法的理论与实验研究[J]. 无机材料学报, 2009, 24(5): 924-928.
[15]	王殿元,王庆凯,常章用,郭艳艳,吴杏华. Y₂Zr₂O₇∶Eu³⁺纳米微粒的合成与变温发光特性研究[J]. 无机材料学报, 2009, 24(2): 239-242.