AlN-BN复相陶瓷的热等静压制备与性能研究

doi:10.15541/jim20150501

摘要/Abstract

摘要：

以氮化铝(AlN)和氮化硼(BN)为原料, 无烧结助剂、热等静压烧结制备了AlN-BN复相陶瓷, 研究了热等静压温度和压强对两种不同原料配比(摩尔比)烧结试样的微观结构和性能的影响。结果表明: 增加BN的添加量对复相陶瓷的烧结致密化影响较小, 但逐渐降低硬度和热导率、增大体积电阻率。相同原料配比下, 复相陶瓷的密度越高, 其热导率、体积电阻率、硬度越高。热导率和体积电阻率的实测值与两相复合模型方程较为符合。当n_AlN:n_BN=75:25时, 在温度为1600℃、压强为90 MPa、保温3 h的热等静压工艺下可以制备出相对密度达98.03%、热导率为77.29 W/(m·K)、体积电阻率为1.35×10¹⁵Ω·cm的复相陶瓷。

关键词: AlN-BN复相陶瓷, 热等静压, 热导率, 体积电阻率

Abstract:

AlN-BN composites were fabricated by hot isostatic pressing (HIP) without sintering aid, using aluminum nitride (AlN) and boron nitride (BN) powders as raw materials. The effects of HIP temperature and pressure on microstructure and properties of composites with two different raw material ratios (molar ratio) were investigated. The results show that increasing amount of BN has little impact on densification, but decreases the hardness and thermal conductivity while increases the volume resistivity. The higher the density of the composite is, the higher thermal conductivity, volume resistivity and hardness are. The thermal conductivity and volume resistivity values conform the formula: . AlN-BN composites with the ratio of n_AlN:n_BN = 75:25 were prepared at 1600 ℃, 90 MPa and a dwell time of 3 h by HIP, achieving density of 98.03%, thermal conductivity of 77.29 W/(m·K) and a volume resistivity of 1.35 × 10¹⁵Ω·cm.

Key words: AlN-BN composite ceramics, HIP, thermal conductivity, volume resistivity

中图分类号:

TB332

彭旭, 朱德贵, 李杨绪, 周加敏, 吕振, 郭鹏超. AlN-BN复相陶瓷的热等静压制备与性能研究[J]. 无机材料学报, 2016, 31(5): 535-541.

PENG Xu, ZHU De-Gui, LI Yang-Xu, ZHOU Jia-Min, LV Zhen, GUO Peng-Chao. Fabrication and Property of AlN-BN Composites by Hot Isostatic Pressing[J]. Journal of Inorganic Materials, 2016, 31(5): 535-541.

图/表 10

图1 AlN-BN复相陶瓷的XRD图谱

Fig. 1 XRD patterns of AlN-BN composite ceramics

表1 AlN-BN复相陶瓷的制备工艺与致密度和显微硬度

Table 1 Relative density and hardness of AlN-BN composite ceramics prepared by different HIP processes

n_AlN:n_BN	Sample number	Temperature/℃		Relative density/%	Vickers hardness/GPa
75:25	1#	1550	80	95.01±0.05	2.89±0.08
	2#	1550	120	96.21±0.03	3.15±0.13
	3#	1600	90	98.03±0.05	3.69±0.09
50:50	4#	1550	80	95.46±0.03	1.13±0.15
	5#	1550	120	96.70±0.06	1.65±0.12
	6#	1600	90	97.98±0.08	1.84±0.10

图2 AlN、BN粉末的SEM照片

Fig. 2 SEM images of AlN (a) and BN powders (b)

图3 AlN-BN复相陶瓷断口的SEM照片和EDS图谱

Fig. 3 SEM morphologies and EDS patterns of AlN-BN composites (a) 2#; (b) 5#; (c) 3#; (d) 6#; (e) 3#EDS; (f) 6#EDS

图4 不同厚度的AlN-BN复相陶瓷热导率曲线

Fig. 4 Thermal conductivity vs sample thickness curves of AlN - BN composite ceramics

表2 AlN-BN复相陶瓷的热导率和体积电阻率

Table 2 Thermal conductivity and volume resistivity of AlN-BN composite ceramics

Sample number	Thermal conductivity/ (W·m^-1·K^-1)	Volume resistivity/ (Ω·cm)
1#	57.39	8.40×10¹⁴
2#	68.10	1.10×10¹⁵
3#	77.29	1.35×10¹⁵
4#	40.21	7.73×10¹⁶
5#	40.11	9.15×10¹⁶
6#	51.65	1.18×10¹⁷

图5 致密度对AlN-BN复相陶瓷热导率和体积电阻率的影响

Fig. 5 The influence of the density of AlN-BN composite ceramics on thermal conductivity and volume resistivity

图6 不同厚度AlN-BN复相陶瓷体积电阻率曲线

Fig. 6 Volume resistivity vs sample thickness curves of AlN-BN composite ceramics

图7 AlN-BN复相陶瓷理论与实际热导率

Fig. 7 Theoretical and practical thermal conductivity of AlN-BN composite ceramics

图8 AlN-BN复相陶瓷理论与实际体积电阻率

Fig. 8 Theoretical and practical volume resistivity of AlN-BN composite ceramics

参考文献 21

[1]	WANG QI, CUI WEI, GE YI-YAO, et al.Carbothermal synthesis of spherical AlN granules: effects of synthesis parameters and Y2O3 additive.Ceramics International, 2015, 41(5): 6715-6721.
[2]	TIAN ZHUO, DUAN XIAO-MING, YANG ZHI-HUA, et al. Effects of AlN content on the thermal properties and thermal shock resistance of BN matrix composite ceramic.Journal of Inorganic Materials, 2014(5): 503-508.
[3]	TIAN ZHUO, DUAN XIAO-MING, YANG ZHI-HUA, et al.Ablation mechanism and properties of insitu SiAlON reinforced BN-SiO2 ceramic composite under an oxyacetylene torch environment.Ceramics International, 2014, 40(7): 11149-11155
[4]	FIRESTEIN KONSTANTIN L, STEINMAN ALEXANDERE, GOLOVIN IGORS, et al.Fabrication, characterization, and mechanical properties of spark plasma sintered Al-BN nanoparticle composites.Materials Science and Engineering, 2015, 642: 104-112.
[5]	ZHAO HAI-YANY, WANG WEI-MING, FU Z HENG-YI, et al. Effect of combined additives of CaF2-Y2O3 on microstructrue and thermal conductivity of AlN-BN composite ceramics.Journal of Inorganic Materials, 2008(5): 496-500.
[6]	CHO WONG-SEUNG, CHO MYEONG-WOO, LEE J AE- HYUNG, et al. Effects of h-BN additive on the microstructure and mechanical properties of AlN-based machinable ceramics.Materials Science and Engineering, 2006, 418: 61-67.
[7]	ZHAO HAI-YANG, WANG WEI-MING, FU ZHENG-YI, et al.Thermal conductivity and dielectric property of hot-pressing sintered AlN-BN ceramic composites. Ceramics International, 2009, 35(1): 105-109.
[8]	LI YONG-LI, ZHANG JIAN, ZHANG JIU-XING, et al.Fabrication and thermal conductivity of AlN/BN ceramics by spark plasma sintering.Ceramics International, 2009, 35(6): 2219-2224.
[9]	KUSUNOSE TAKAFUMI, SEKINO TOHUR, ANDO YOICHI, et al.Fabrication of machinable AlN-BN composites with high thermal conductivity by pressureless sintering turbostatic BN-coated AlN nanocomposite powders.Journal of Materials Research, 2008, 23(1): 236-244.
[10]	QIN MING-LI, QU XUAN-HUI, DUAN BO-HAI, et al. No pressure sintering high density AlN-BN composite ceramics.Journal of Inorganic Materials, 2005(1): 245-250.
[11]	WU YU-BIAO, ZHAN JUN, ZHANG HAO, et al.Present situation on low temperature sintering additives of high thermal conductivity AlN ceramics.China Ceramics, 2013, 9: 2.
[12]	KANAI TAKAO, TANEMOTO KEI, KUBO HIROSHI, et al.Reaction -bonded boron nitride-aluminum nitride ceramic composites.Japanese Journal of Applied Physics. 1991, 30: 1235.
[13]	BOCANEGRA M H.Hot isostatic pressing (HIP) technology and its applications to metals and ceramics.Journal of Materials Science, 2004, 39: 6399-6420.
[14]	DADBAKHSH S, HAO L.Effect of hot isostatic pressing (HIP) on Al composite parts made from laser consolidated Al/Fe2O3 powder mixtures.Journal of Materials Processing Technology, 2012, 212(11): 2474-2483.
[15]	YE NAI-QINQ, ZENG ZHAO-QIANG.The main obstacle BN matrix composite densification.Modern Technical Ceramics, 1998 (1): 10-22.
[16]	KIM W.Morphological effect of second phase on thermal conduetivity of AlN ceramics.J. Am. Ceramic Soc., 1996, 79(4): 1066-1072.
[17]	TAJIKA M, MATSUBARA H, RAFANIELLO W, et al.Effect of grain contiguity on the thermal diffusivity of aluminum nitride.J. Am. Ceramic Soc., 1999, 82(6): 1573-1575.
[18]	WANG DE-MIN.Moist air conducting it?Wuxi Education Journals, 2001(3): 79-80.
[19]	魏錾钉. AlN/nano-BN复相陶瓷的SPS制备与性能研究. 武汉: 武汉理工大学硕士学位论文, 2007.
[20]	BELOVA I V, MURCH E, MONTE C, et al. Simulation of the effective thermal conductivity in two-phase material. Journal of Materials Processing Technology, 2004, 153-154: 741-745.
[21]	LI FA, LIU ZHENG.High thermal conducitivy AlN ceramic materials and its application research.Vacuum Electronic Technology, 2002(3): 56-58.
	ZHOU WEN-YING, QI SHU-HUA, WU YOU-MING, et al. BN/HDPE thermal conductivity of thermal conductive plastic.Ploymer Materials Science And Engineering, 2008(02): 83-86