Mechanical Properties and Thermal Conductivity of Si3N4 Ceramics with Composite Sintering Additives

doi:10.15541/jim20220101

Abstract

Abstract:

Si₃N₄ceramics have become one of the most promising materials for third-generation semiconductor’s ceramic substrates due to its excellent mechanical and thermal properties. In this work, seven rare earth oxides (RE₂O₃, RE=Sc, Lu, Yb, Y, Gd, Nd, La) and non-oxides (MgSiN₂) were used as composite sintering additives to prepare Si₃N₄ ceramics with high strength and high thermal conductivity by hot pressing sintering and annealing. The effects of RE₂O₃ types in the composite additives on the phase composition, microstructure, mechanical properties, and thermal conductivity of Si₃N₄ ceramics were systematically studied. The mechanical properties of Si₃N₄ ceramics after hot pressing sintering were superior to that without hot pressing, and the bending strength of the sample with Nd₂O₃-MgSiN₂ additive reached (1115±49) MPa. After annealing, the thermal conductivity of Si₃N₄ceramics increased significantly, and gradually increased with the decrease of the rare earth ion’s radius. The thermal conductivity of the sample with Sc₂O₃-MgSiN₂ additive increased from 54.7 W·m^-1·K^-1to 80.7 W·m^-1·K^-1 (increased by 47.6%) after annealing. The results indicate that Sc₂O₃-MgSiN₂is expected to be a new composite additive for the preparation of high strength and high thermal conductivity Si₃N₄ceramics as compared to the internationally accepted combination of Y₂O₃-MgSiN₂ and Yb₂O₃-MgSiN₂ additives.

Key words: silicon nitride, composite sintering additives, annealing, thermal conductivity

CLC Number:

TQ174

FU Shi, YANG Zengchao, LI Honghua, WANG Liang, LI Jiangtao. Mechanical Properties and Thermal Conductivity of Si₃N₄ Ceramics with Composite Sintering Additives[J]. Journal of Inorganic Materials, 2022, 37(9): 947-953.

Figures/Tables 7

Fig. 1 XRD patterns of Si3N4 ceramics with different additive systems prepared by hot pressing sintering

Fig. 2 SEM images of the polished surfaces of Si3N4 ceramics with different additive systems prepared by hot pressing sintering (a) LuM; (b) YbM; (c) YM; (d) GdM; (e) NdM; (f) LaM

Table 1 Properties of Si3N4 ceramic samples prepared by hot pressing sintering

Sample	Ionic radius/nm	Relative density/%	Grain size/μm	Vickers’ hardness/GPa	Flexural strength/MPa	Fracture toughness/ (MPa·m^1/2)	Thermal conductivity/ (W·m^-1·K^-1)
ScM	0.073	99.36	0.72±0.32	14.58±0.25	905±36	8.21±0.09	54.7
LuM	0.085	99.53	0.9±0.40	14.75±0.20	785±25	8.01±0.12	49.6
YbM	0.086	99.49	0.97±0.47	14.75±0.27	759±20	8.03±0.16	49.7
YM	0.089	99.73	1.03±0.46	14.64±0.29	819±10	8.65±0.11	51.1
GdM	0.094	99.89	1.01±0.48	14.57±0.22	792±34	7.62±0.47	54.6
NdM	0.100	99.37	0.95±0.42	14.79±0.27	1115±49	7.19±0.10	53.9
LaM	0.106	99.21	0.9±0.41	15.37±0.33	978±39	7.25±0.10	52.8

Fig. 3 XRD patterns of Si3N4 ceramics with different additive systems after annealing

Fig. 4 SEM images of the polished surfaces of Si3N4 ceramics with different additive systems after annealing (a) LuMH; (b) YbMH; (c) YMH; (d) GdMH; (e) NdMH; (f) LaMH

Fig. 5 (a) Average grain size, (b) bending strength, (c) fracture toughness, and (d) thermal conductivity changing with radius of rare earth ion of Si3N4 ceramics before and after annealing

Fig. 6 Microstructures of Si3N4 ceramic samples before and after annealing (a) ScM and (d) ScMH etched by molten NaOH; Fracture surfaces of (b) YM, (e) YMH, (c) YbM and (f) YbMH

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Mechanical Properties and Thermal Conductivity of Si₃N₄ Ceramics with Composite Sintering Additives

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