镁铝合金直接燃烧法合成AlN晶体

doi:10.15541/jim20180244

摘要/Abstract

摘要：

以球形镁铝合金(Al₁₂Mg₁₇)颗粒为原料, 在空气中直接燃烧合成氮化铝(AlN)晶体。实验样品堆积在直径为 1 cm的区域内, 使用乙烷火焰点燃。使用高速摄像仪记录燃烧合成过程。借助XRD和SEM对原料和产物的组成及结构进行分析, 并使用TG-DSC分析合金的热力学性质。结果表明: 镁铝合金中的铝可以全部转化为AlN晶体。合金的点火温度约为494.4 ℃, 一旦点燃, 不需要外界热源的持续加热, 样品可持续燃烧。燃烧开始后, 合金颗粒中镁快速汽化, 与空气中氧发生优先反应, 并耗掉颗粒周围的氧气, 使氮气进入液态铝表层, 生成氮化铝。燃烧产物有明显分层, 检测结果表明上层产物为白色氧化镁, 下层产物为黑色氮化铝晶体。合成过程中, 镁对氮化铝的形成起着积极的促进作用。

关键词: AlN, 镁铝合金, 燃烧

Abstract:

Aluminum nitride (AlN) was synthesized by direct combustion of spherical Mg-Al alloy powder in air. The alloy (Al₁₂Mg₁₇) heaped up within a heating area (1 cm in diameter) and was ignited by butane flame. Synthetic process was recorded by a high-speed camera. Morphology and phase makeup of initial powder and combustion products were analyzed by scanning electron microscope and X-ray diffraction. Thermodynamic property of the alloy was analyzed using TG-DSC. The results show that the Al in the Mg-Al alloy powder can be completely transformed to AlN. Ignition temperature of the alloy is about 494.4℃. Once the alloy powder is ignited, self-sustained combustion in the powder can be observed. When combustion begins, Mg can rapidly vaporize and react with oxygen. This oxidation reaction can consume the oxygen around the particles, leading N₂ diffusing to the liquid Al layer. Combustion products of the alloy consist of two different layers.The upper white layer contains only MgO and the lower black layer contains only AlN. During synthetic process, the existence of Mg significantly promotes the nitridation of Al.

Key words: AlN, Mg-Al alloy, combustion

中图分类号:

TQ174

谢晓, 隋颖, 黄晓昱, 朱晨光. 镁铝合金直接燃烧法合成AlN晶体[J]. 无机材料学报, 2019, 34(4): 439-443.

Xiao XIE, Yin SUI, Xiao-Yu HUANG, Chen-Guang ZHU. Synthesis of AlN by Direct Combustion of Mg-Al Alloy Powder[J]. Journal of Inorganic Materials, 2019, 34(4): 439-443.

图/表 8

表1 实验使用的主要仪器设备及其生产厂家

Table 1 Main instruments used in the test and their manufactures

Instrument	Model	Manufacture
Laser fineness gage	BT-9300H	Bettersize
Scanning Electron Microscope(SEM)	JEOLJSM 6500F	JEOL
Thermogravimetric Analysis and Differential Scanning Calorimeter(TG-DSC)	STA449F3	NETZSCH
X-ray Diffractometer (XRD)	D8	Bruker
High-speed camera	MotionXtra HG-100K	READLAKE

图1 镁铝合金性质分析

Fig. 1 Analysis of the Mg-Al alloy powder (a) XRD pattern; (b) Size distribution; (c) SEM image; (d) Magnified area in (c)

图2 镁铝合金在空气环境下的TG-DSC曲线

Fig. 2 TG-DSC curves for Mg-Al alloy heated in air

图3 使用高速摄像仪记录的镁铝合金粒子在空气中的燃烧过程。

Fig. 3 Combustion process of Mg-Al alloy in air recorded by a high-speed camera

图4 镁铝合金在空气中的燃烧产物

Fig. 4 Combustion products of Mg-Al alloy particles burned in air

图5 镁铝合金在空气中的燃烧产物的XRD图谱

Fig. 5 XRD patterns of the combustion products of the Mg-Al alloy particles in air (a) Upper white oxide; (b) Lower black material

图6 镁铝合金在空气中燃烧产生的AlN颗粒(a) 和AlN晶须(b)的SEM照片

Fig. 6 SEM images of AlN particles (a) and AlN whiskers (b) formed when the Mg-Al alloy powder was burned in air

图7 镁铝合金在空气中燃烧合成AlN的机理

Fig. 7 Synthetic mechanism of AlN by direct combustion of Mg-Al alloy in air

参考文献 14

[1]	HE YONG-QIN, LI XIAO-YUN, ZHANG JING-XIAN , et al. In situ pyrolyzed carbon on the property of AlN-based microwave attenuation ceramics. Journal of Inorganic Materials, 2018,33(4):421-426.
[2]	LEE CHING-SUNG, HSU WEI-CHOU, LIU HAN-YIN , et al. Al₂O₃-dielectric In_0.18Al_0.82N/AlN/GaN/Si metal-oxide-semi- conductor heterostructure field-effect transistors with backside substrate metal-trench structure. IEEE Journal of the Electron Devices Society, 2017,6(1):68-73.
[3]	WANG CHENG, LI JI-SHENG, XU LIANG-GE , et al. Preparation of aluminum nitride ceramic circuit substrate with double-edged heterogeneous treatment. China Ceramics, 2018,54(1):50-55.
[4]	WANG JIE, ZHANG ZHAN-YING, LÜ XIN-LÜ . Current research status and prospect of synthesis methods of aluminum nitride powder. Bulletin of the Chinese Ceramic Society, 2010,29(5):1098-1102.
[5]	RADWAN M, BAHGAT M . A modified direct nitridation method for formation of nano-AlN whiskers. Journal of Materials Processing Tech, 2007,181(1):99-105.
[6]	RADWAN M, BAHGAT M, EL-GEASSY A A. Formation of aluminum nitride whiskers by direct nitridation. Journal of the European Ceramic Society, 2006,26(13):2485-2488.
[7]	陈淑文 . AlN粉体的合成与烧结机制研究. 杭州: 浙江工业大学硕士学位论文, 2015.
[8]	WU HAO-YANG, QIN MING-LI, CHU AI-MIN , et al. AlN powder synthesis by sodium fluoride-assisted carbothermal combustion. Ceramics International, 2014,40(9):14447-14452.
[9]	GROMOV A, VERESHCHAGIN V . Study of aluminum nitride formation by superfine aluminum powder combustion in air. Journal of the European Ceramic Society, 2004,24(9):2879-2884.
[10]	MOSTOVSHCHIKOV A V, ILYIN A P, SHMAKOV A N , et al. Investigation of the aluminum nitride formation during the aluminum nanopowder combustion in air. Physics Procedia, 2016,84:302-306.
[11]	ALY Y, DREIZIN E L . Ignition and combustion of Al·Mg alloy powders prepared by different techniques. Combustion & Flame, 2015,162(4):1440-1447.
[12]	SHIH T S, WANG J H, CHONG K Z . Combustion of magnesium alloys in air. Materials Chemistry & Physics, 2004,85(2):302-309.
[13]	NIE H, SCHOENITZ M, DREIZIN E L . Oxidation of differently prepared Al-Mg alloy powders in oxygen. Journal of Alloys & Compounds, 2016,685:402-410.
[14]	POPENKO E M, GROMOV A A, PAUTOVA Y I , et al. SEM-EDX study of the crystal structure of the condensed combustion products of the aluminum nanopowder burned in air under the different pressures. Applied Surface Science, 2011,257(8):3641-3644.

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