泡沫前驱体碳热还原氮化法合成氮化铝粉体

doi:10.15541/jim20170067

无机材料学报 ›› 2017, Vol. 32 ›› Issue (10): 1115-1120.DOI: 10.15541/jim20170067 CSTR: 32189.14.10.15541/jim20170067

• • 上一篇

泡沫前驱体碳热还原氮化法合成氮化铝粉体

茅茜茜^1,2,3, 李军¹, 张海龙², 徐勇刚^1,2,3, 王士维^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. 中国科学院上海硅酸盐研究所, 中国科学院光功能无机材料重点实验室, 上海 200050; 3. 中国科学院大学, 北京 100039)

收稿日期:2017-02-10 出版日期:2017-10-20 网络出版日期:2017-09-21
作者简介:茅茜茜. E-mail: 112113192@qq.com

Synthesis of AlN Powder by Carbothermal Reduction-nitridation of Alumina/Carbon Black Foam

MAO Xi-Xi^1,2,3, LI Jun¹, ZHANG Hai-Long², XU Yong-Gang^1,2,3, WANG Shi-Wei^1,2

(1. State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China; 2. Chinese Academy of Sciences Key Laboratory of Transparent and Opto-functional Advanced Inorganic Materials, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China; 3. University of Chinese Academy of Sciences, Beijing 100039, China)

Received:2017-02-10 Published:2017-10-20 Online:2017-09-21
About author:MAO Xi-Xi(1991-), female, candidate of Master degree. E-mail: 112113192@qq.com

摘要/Abstract

摘要：

本研究采用碳热还原氮化法(CRN)合成AlN粉体。以γ-Al₂O₃和炭黑为原料, 采用直接发泡工艺与注凝成型相结合的方法制备出Al₂O₃/C泡沫, 作为合成AlN粉体的前驱体。泡沫孔隙尺寸从几十微米到几百微米, 总孔隙率56%~90%。具有通孔结构的泡沫前驱体实现了原料内部各处的均匀的固-气反应, 泡沫总孔隙率≥80%可显著提高CRN反应的速率。XRD分析结果显示: CRN过程中存在γ-Al₂O₃到α-Al₂O₃的相转变, 反应起始温度在1300℃以上, 并在1550℃反应完全。在1650℃合成得到的AlN颗粒平均粒径不超过1 µm, 氮含量为32.9wt%。

关键词: 化学制备, 孔隙率, 碳热还原, 氮化铝

Abstract:

Alumina/carbon black foam was prepared by mechanical foaming and aqueous gelcasting and used as precursor for the production of AlN powder. The foam with large open pores ensures homogeneous solid-gas reaction during carbothermal reduction-nitridation (CRN) process. Further, the solid-gas contact is enlarged by oppositely feeding the foam and nitrogen in a vertical furnace. Solid-gas reaction efficiency of the CRN process was greatly enhanced when total porosity of the foam was ≥80%. XRD results revealed that γ-Al₂O₃ transformed to α-Al₂O₃ and then was carbothermal reduction-nitridationed to be AlN phase. AlN powder with an average particle size of less than 1 µm was synthesized at 1650℃ and contained 32.9wt% nitrogen.

Key words: chemical preparation, porosity, carbothermal reduction, aluminum nitride

中图分类号:

TQ174

茅茜茜, 李军, 张海龙, 徐勇刚, 王士维. 泡沫前驱体碳热还原氮化法合成氮化铝粉体[J]. 无机材料学报, 2017, 32(10): 1115-1120.

MAO Xi-Xi, LI Jun, ZHANG Hai-Long, XU Yong-Gang, WANG Shi-Wei. Synthesis of AlN Powder by Carbothermal Reduction-nitridation of Alumina/Carbon Black Foam[J]. Journal of Inorganic Materials, 2017, 32(10): 1115-1120.

图/表 10

Fig. 1 Effect of dispersant on the Zeta potential of alumina and carbon black slurry

Fig. 2 Rheological behavior of Al2O3/C slurries with different solids loading and dispersant content

Fig. 3 Evolution of the foaming capacity versus surfactant content

Fig. 4 SEM micrographs of porous Al2O3/C foams with different surfactant additions(a) 0vol%; (b) 2.0vol%; (c) 2.4vol%; (d) 4.0vol%

Fig. 5 Effects of surfactant content on total porosity and open-pore ratio of foams

Fig. 6 Effect of porosity on nitridation rate under 1600℃

Fig. 7 XRD patterns of the products by heating Al2O3/C foams at different temperatures

Fig. 8 SEM micrographs of foam with addition of 2.4vol% surfactant before (a) and after (b) being calcined at 1300℃ for 2 h

Fig. 9 SEM photographs of AlN powders synthesized at different temperatures for 2 h(a) 1550℃; (b) 1600℃; (c) 1650℃

Table 1 Nitrogen and oxygen content of AlN powder synthesized at different temperatures

Element content/wt%	Reaction temperature/℃
Element content/wt%	1550	1600	1650
Nitrogen	31.9	32.4	32.9
Oxygen	1.6	1.2	1.1

参考文献 20

[1]	SELVADURAY G, SHEET L.Aluminium nitride: review of synthesis methods.Mater. Sci. Technol., 1993, 9(6): 463-473.
[2]	BACHELARD R, JOUBERT P.Aluminum nitride by carbothermal reduction.Mater. Sci. Eng. A, 1989, 109: 247-251.
[3]	VIRKAR ANIL V, JACKSON T BARRETT, CUTLER RAYMOND.Thermodynamic and kinetic effects of oxygen removal on the thermal conductivity of aluminum nitride.J. Am. Ceram. Soc., 1989, 72(11): 2031-2042.
[4]	WEI P, QING Y, JUAN C.Mechanism of carbothermal synthesis of aluminium nitride.Thermochim Acta, 1999, 325(1): 89-93.
[5]	WANG Q, GE Y Y, CUI W, et al.Carbothermal synthesis of micro-scale spherical AlN granules with CaF2 additive.J. Alloys Compd., 2016, 663: 823-828.
[6]	IDE T, KOMEYA K, MEGURO T, et al.Synthesis of AlN powder by carbothermal reduction-nitridation of various Al2O3 powders with CaF2.J. Am. Ceram. Soc., 1999, 82(11): 2993-2998.
[7]	MOLISANI A L, YOSHIMURA H N.Low-temperature synthesis of AlN powder with multicomponent additive systems by carbothermal reduction-nitridation method.Mater. Res. Bull., 2010, 45(6): 733-738.
[8]	ZAKORZHEVSKII V V, BOROVINSKAYA I P, SACHKOVA N V.Combustion synthesis of aluminum nitride.Inorg. Mater., 2001, 38(11): 1131-1140.
[9]	CHU A, QIN M, JIA B, et al.Citric acid-assisted combustion- carbothermal synthesis of well-distributed highly sinterable AlN nanopowders.J. Am. Ceram. Soc., 2012, 95(8): 2510-2515.
[10]	WANG Q, CUI W, GE Y Y, et al.Preparation of spherical AlN granules directly by carbothermal reduction-nitridation method.J. Am. Ceram. Soc., 2015, 98(2): 392-397.
[11]	LI C, KAO L, CHEN M, et al.Rapid preparation of aluminum nitride powders by using microwave plasma.J. Alloys Compd., 2012, 542: 78-84.
[12]	CHU A, QIN M, JIA B, et al.Effect of urea on the size and morphology of AlN nanoparticles synthesized from combustion synthesis precursors. J. Alloys Compd., 2012, 530: 144-151.
[13]	LEE S H, YI J H, KIM J H, et al.Preparation of nanometer AlN powders by combining spray pyrolysis with carbothermal reduction and nitridation.Ceram. Int., 2011, 37(6): 1967-1971.
[14]	KOMEYA K.Synthesis of AlN Powder by carbothermal reduction- nitridation method.J. Ceram. Soc. Jpn., 1993, 101(4): 377-382.
[15]	YANG Y, SHIMAI S, SUN Y, et al.Fabrication of porous Al2O3 ceramics by rapid gelation and mechanical foaming.J. Mater. Res., 2013, 28(15): 2012-2016.
[16]	ZHANG X, SUN Y, SHIMAI S, et al.Effect of water-soluble epoxy resin on microstructure and properties of porous alumina ceramics by gel-casting.J. Inorg. Mater., 2015, 30(10): 1085-1088.
[17]	SEPULVEDA P, BINNER J G B. Processing of cellular ceramics by foaming and in situ polymerisation of organic monomers.J. Eur. Ceram. Soc., 1999, 19(12): 2059-2066.
[18]	YANG Y, SHIMAI S, WANG S.Room-temperature gelcasting of alumina with a water-soluble copolymer.J. Mater. Res., 2013, 28(11): 1512-1516.
[19]	SUN Y, SHIMAI S, PENG X, et al.A method for gelcasting high-strength alumina ceramics with low shrinkage.J. Mater. Res., 2014, 29(2): 247-251.
[20]	MAO X, SHIMAI S, WANG S.Gelcasting of alumina foams consolidated by epoxy resin.J. Eur. Ceram. Soc., 2008, 28(1): 217-222.

泡沫前驱体碳热还原氮化法合成氮化铝粉体

Synthesis of AlN Powder by Carbothermal Reduction-nitridation of Alumina/Carbon Black Foam

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