A general strategy towards improving the strength and thermal shock resistance of glass-ceramics through microstructure regulation

doi:10.1016/j.jmst.2022.03.001

摘要/Abstract

Abstract:

Glass-ceramics are usually obtained through controlled crystallization. In this work, we propose a new strategy to add an appropriate amount of oxide particles to the parent glass to improve the performance of glass-ceramics. Different amounts of Al₂O₃ or/and CeO₂ particles were added into a SiO₂-Al₂O₃-ZnO-CaO-ZrO₂-TiO₂ based glass, and crystallization behavior, fracture strength, and thermal shock behavior were systematically evaluated. The results indicate that with the addition of Al₂O₃ or/and CeO₂ particles of moderate amount, the unfavorable needle-like ZrSiO₄, Zn₂SiO₄, and CaTiSiO₅ crystals were largely inhibited when annealed at 900 °C. Accordingly, fracture strength is maintained high after heating at high temperatures. The thermal shock resistance is also enhanced drastically. The additive Al₂O₃ is thermodynamically favorable to react with the glass, forming particulate ZnAl₂O₄ instead of precipitating the needle-like crystals of Zn₂SiO₄ and CaTiSiO₅; while CeO₂ will combine with ZrO₂ to form a solid solution and promote the precipitation of primary crystal CaZrTi₂O₇ that will not transform to ZrSiO₄ with prolonging thermal exposure.

Key words: Non-metallic glasses (silicates), Crystallization, MicrostructureMechanical property, High-temperature oxidation

. [J]. 材料科学与技术, 2022, 120(0): 139-149.

Min Feng, Chengyang Jiang, Minghui Chen, Shenglong Zhu, Fuhui Wang. A general strategy towards improving the strength and thermal shock resistance of glass-ceramics through microstructure regulation[J]. J. Mater. Sci. Technol., 2022, 120(0): 139-149.

图/表 13

Table 1. Nominal composition of the glass-ceramics (wt.%).

SiO₂	Al₂O₃	ZnO	CaO	ZrO₂	TiO₂	B₂O₃	Na₂O	KNO₃
58.26	5.98	9.00	3.66	5.29	2.75	4.66	3.40	7.00

Fig. 1. (a) XRD patterns of glass-ceramics PE, E25A, E25C, and E10A15C after annealing at 900 °C for 5 min, 0.5, and 10 h; (b) SEM microstructures after annealing for 0.5 h; (c) SEM microstructures after annealing for 10 h.

Fig. 2. (a-c) XRD patterns of glass-ceramics with the addition of Al2O3 or/and CeO2 after annealing at 900 °C for 10 h; (d) variation of contents of Zn2SiO4 and CaTiSiO5 with Al2O3 addition; (e) variation of contents of ZrSiO4 with the addition of CeO2; (f) variation of contents of all needle-like crystals with the addition of Al2O3 or/and CeO2 (the red line represents Zn2SiO4 and CaTiSiO5, and the blue line represents ZrSiO4).

Fig. 3. (a) TEM microstructure and elemental maps of PE annealed at 900 °C for 0.5 h; (b) and (c) SAED patterns obtained at areas “1” and “2” in (a), respectively.

Table 2. EDS analysis at different zones in Fig. 3(a) (at.%).

Zone	O	Si	Ca	Ti	Zr	Others
1	51.6	0.5	5.9	16.3	20.9	4.8
2	47.5	24.8	6.7	9.4	9.6	2.0
3	37.9	60.3	0.2	-	0.7	0.9

Fig. 4. (a) TEM microstructure and elemental maps of E25A annealed at 900 °C for 0.5 h; (b) and (c) HRTEM images of the zones “1” and “2” in (a), respectively. Insets are Fast Fourier Transform (FFT) electron diffraction patterns.

Fig. 5. (a, b) TEM microstructures and elemental maps of E25C annealed at 900 °C for 0.5 h; (c, d) HRTEM images at the interface between zones “1” and “2” in (b). Insets are Fast Fourier Transform (FFT) electron diffraction patterns.

Table 3. EDS analysis at different zones in Fig. 5(b) (at.%).

Zone	O	Si	Ca	Ti	Zr	Ce	Others
1	62.1	19.7	0.9	0.5	2.9	13.5	0.4
2	59.7	8.2	6.1	8.5	8.0	2.1	7.4
3	57.1	36.1	0.3	-	1.2	-	5.3

Fig. 6. (a) Fracture strength of glass-ceramics E10A, E10A5C, E10A10C, and E10A15C as a function of annealing time; (b) fracture surface morphologies of glass-ceramics corresponding to Ⅰ, Ⅱ, Ⅲ, and Ⅳ in (a).

Fig. 7. (a) Mass change of glass-ceramic coatings PE, E25A, E25C, E10A15C, and E15A10C after thermal shock at 900 °C for different cycles (inset is the enlarged view); (b) macro morphologies of different glass-ceramic coatings after thermal shock for 0,10, and 50 cycles.

Fig. 8. Surface morphologies and cross-sectional microstructures of the glass-ceramic coatings: (a, e) PE; (b, f) E25A, (c, g) E25C, and (d, h) E10A15C after thermal shock at 900 °C for 50 cycles.

Table 4. Thermo-physical properties of ZrSiO4, Zn2SiO4, and glass.

Materials	CTE (10^-6/°C)	Young's moduli (GPa)	Poisson's ratios	Shear moduli (GPa)	Bulk moduli (GPa)
ZrSiO₄	4.99 [35]	27 [36]	0.27 [37]	107	196
Zn₂SiO₄	2.80 [38]	12 [39]	0.30 [40]	50	108
Glass	5.70 [41]	72 [41]	0.29 [40]	28	57

Fig. 9. Variations of thermal stress developed in glass with volume fraction of precipitates (a) ZrSiO4 and (b) Zn2SiO4 during cooling.

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