Preparation and Thermal Stability of Ti3SiC2 Ceramics by Polymer Derived Ceramics Method

doi:10.15541/jim20240013

Abstract

Abstract:

Ti₃SiC₂ compound can enhance the oxidation resistance of C/C composites as a modifying material, thanks for its superior high-temperature stability, indicating significant potential for applications. In this work, titanium powder and liquid polycarbosilane (LPCS) were served as starting materials for producing Ti₃SiC₂ ceramics with four different phase contents by polymer derived ceramics (PDC) method at temperatures of 1200, 1300, 1400, and 1500 ℃, respectively. Effects of sintering temperature on the phase compositions and morphology of the ceramics were studied. Additionally, the impact of varying Ti₃SiC₂ phase contents on oxidation resistance and thermal shock resistance were also explored. The results showed that layered Ti₃SiC₂ formed at Ti : Si molar ratio of 3 : 1.5 when sintered at 1300, 1400, and 1500 ℃, respectively. After sintered at 1400 ℃, the mass fraction of Ti₃SiC₂ in the ceramic product reached 92.10% with the bending strength of 172.68 MPa. When subjected to a static air environment of 1300 ℃ for 7 h, the oxidation weight of the ceramics obtained progressively reduction with the increase of Ti₃SiC₂ phase content. During the oxidation process, a protective film primarily consisted of TiO₂ was formed on the surface, which effectively slowed down the oxygen diffusion into the interior. Air thermal shock tests at 1300 ℃ and flexural strength assessments demonstrated that the residual strength of all materials decreased with the increase of thermal shock times. Nevertheless, the thermal shock resistance and residual strength of the samples were enhanced with the increase of Ti₃SiC₂ phase content. After 30 times thermal shock, the sample with the mass fraction of Ti₃SiC₂ phase of 92.10% experienced 30.66% weight loss and retained residual strength of 120.18 MPa, primarily due to the layered structure of Ti₃SiC₂ which is significantly extends the crack propagation path and its superior oxidation resistance.

Key words: Ti₃SiC₂, pressureless sintering, oxidation resistance, thermal shock resistance

CLC Number:

TB34

ZHENG Bin, KANG Kai, ZHANG Qing, YE Fang, XIE Jing, JIA Yan, SUN Guodong, CHENG Laifei. Preparation and Thermal Stability of Ti₃SiC₂ Ceramics by Polymer Derived Ceramics Method[J]. Journal of Inorganic Materials, 2024, 39(6): 733-740.

Figures/Tables 17

Fig.1 XRD patterns of Ti3SiC2 sintered at different temperatures

Table 1 Mass percentages of phases in samples sintered at different temperatures

Group	TiC/%	Ti₅Si₃/%	Ti₃SiC₂/%
A	45.58	54.42	0
B	37.16	45.52	17.32
C	7.90	0	92.10
D	47.97	0	52.03

Fig. 2 SEM images of samples sintered at different temperatures (a) Group A; (b) Group B; (c) Group C; (d) Group D

Table 2 Density and porosity of samples sintered at different temperatures

Group	Density/(g·cm^-3)	Porosity/%
A	1.77	27.52
B	1.62	22.25
C	1.82	18.47
D	1.69	18.53

Fig. 3 Thermogravimetric curves of samples from three groups (a) Group B; (b) Group C; (c) Group D

Fig. 4 Relationships of (a) weight gain per unit surface area and (b) weight gain per unit surface area square with time of three groups after oxidation in air at 1300 ℃

Table 3 Air oxidation rate constants of group B-D at 1300 ℃

Group	K_p/(kg²·m^-4·h^-1)
B	0.8485
C	0.1636
D	0.4399

Fig. 5 SEM images and EDS mappings of the surfaces of three groups (a) Group B; (b) Group C; (c) Group D

Fig. 6 XRD patterns of the oxidized surface of three groups

Fig. 7 Changes of Gibbs free energy in oxidation process

Fig. 8 SEM images and EDS analyses of cross-sections of three groups (a) Group B; (b) Group C; (c) Group D

Table 4 Material mass change rates after different thermal shocks

Group	Mass change rate/%
Group	15 times	30 times
B	37.95	39.34
C	30.09	30.66
D	35.81	36.91

Fig. 9 XRD patterns three groups of samples after 30 thermal shocks

Fig. 10 Three-point flexural load-displacement curves of samples of three groups after different thermal shock times (a) Group B; (b) Group C; (c) Group D

Fig. 11 Bending strengths of samples from three groups after different thermal shock times Colorful figure is available on website

Fig. 12 Macro photos of samples of three groups after different thermal shock times (a) 0 times; (b) 15 times; (c) 30 times

Fig.13 SEM images of a sample from group C after 15 thermal shocks (a) Delamination; (b) Crack deflection

References 17

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Preparation and Thermal Stability of Ti₃SiC₂ Ceramics by Polymer Derived Ceramics Method

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