Rare Earth Oxides on Property of Pressureless Sintered Si3N4 Ceramics

doi:10.15541/jim20170056

Abstract

Abstract:

High thermal conductivity Si₃N₄ ceramic is a prospective substrate material for high-power electronic devices. In this paper, pressureless and liquid-phase sintering was proposed using Re₂O₃ (Re=Sm, Er, Lu) - TiO₂ as sintering additives to effectively reduce the cost for applications. Effect of the additive type and content on microstructure, mechanical properties and thermal conductivity of the ceramic were investigated. Results showed that the relative density, thermal conductivity and grain size of Si₃N₄ decrease gradually with the increase of Re ionic (Re³⁺) radius. With addition of Sm₂O₃, the highest density can only reach 3.14 g/cm³, while the fracture toughness about 5.76 MPa•m^1/2 can be obtained when 8wt% Sm₂O₃-TiO₂ is used. With 12wt% Lu₂O₃-TiO₂ as sintering aid, Si₃N₄ ceramics show high density of 3.28 g/cm³ as well as high fracture toughness, while the thermal conductivity is only 42 W/(m∙K) due to the presence of large amount of second phase. Thermal conductivity of Si₃N₄ reaches 51.8 W/(m∙K) with the addition of 8wt% Er₂O₃-TiO₂, which can meet the requirement for substrate materials for power electronic device.

Key words: rare earth oxide, silicon nitride, thermal conductivity, pressureless sintering

CLC Number:

TQ174

DUAN Yu-Sen, ZHANG Jing-Xian, LI Xiao-Guang, HUANG Ming-Ming, SHI Ying, XIE Jian-Jun, JIANG Dong-Liang. Rare Earth Oxides on Property of Pressureless Sintered Si₃N₄ Ceramics[J]. Journal of Inorganic Materials, 2017, 32(12): 1275-1279.

Figures/Tables 8

Table 1 The mass ratio of Re2O3 to TiO2

	Sm₂O₃:TiO₂(ST)	Er₂O₃:TiO₂(ET)	Lu₂O₃:TiO₂(LT)
Mass ratio	2:1	1:1	1:1

Fig. 1 Variation of density of Si3N4 ceramics with different type and content of sintering additives

Table 2 Ion radius, electronegativity and melting point of rare earth elements

Element	Sm	Er	Lu
Atomic number	62	68	71
Re³⁺radius/pm	95.8	89.0	86.1
Electronegaticity	1.17	1.24	1.27
T_M of Re₂O₃/℃	2262	2387	2510

Fig. 2 XRD patterns of Si3N4 ceramics with different sintering additives type (the sintering additives content was 8wt%) (a) and Si3N4 ceramics with different sintering additive contents (the sintering additive was Sm2O3-TiO2)(b)

Table 3 Mass ratio of β-Si3N4 to TiN

	ST-1	ST-2	ST-3	ST-4
W_β-Si3N4/W_TiN	—	57.8	40.6	30.2

Fig. 3 Variation of thermal conductivity of Si3N4 ceramic with different sintering additives type and content

Fig. 4 Microstructures of Si3N4 ceramic (a)LT-3 and (b)ET-3 with different sintering additives

Table 4 Mechanical properties of Si3N4 ceramic with different sintering additives and the corresponding thermal conductivity value after annealing at 1600℃ for 8 h

Sample	Fracture toughness/ (MPa•m^1/2)	Hardness/ GPa	Thermal conductivity after annealing/ (W∙m^-1∙K^-1)
LT-3	5.29	10.8	45.3
ET-3	5.46	12.2	51.8
ST-3	5.76	11.7	40.8

References 19

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Rare Earth Oxides on Property of Pressureless Sintered Si₃N₄ Ceramics

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