High entropy ultra-high temperature ceramic thermal insulator (Zr1/5Hf1/5Nb1/5Ta1/5Ti1/5)C with controlled microstructure and outstanding properties

doi:10.1016/j.jmst.2021.12.030

Abstract

Abstract:

Due to advancements of hypersonic vehicles, ultra-high temperature thermal insulation materials are urgently requested to shield harsh environment with superhigh heat flux. Toward this target, ultra-high temperature ceramics (UHTCs) are the only choice due to their excellent capability at ultra-high temperatures. We herein report a novel highly porous high entropy (Zr1/5Hf1/5Nb1/5Ta1/5Ti1/5)C fabricated by foam-gelcasting-freeze drying technology combined with in-situ pressureless reaction sintering. The porous (Zr1/5Hf1/5Nb1/5Ta1/5Ti1/5)C exhibited ultra-high porosity of 86.4%-95.9%, as well as high strength and low thermal conductivity of 0.70-11.77 MPa and 0.164-0.239 W/(m⋅K), respectively. Specifically, SiC sintering additive only locates at the pit of the surface of sintering neck between UHTC grains, and there is no secondary phase or intergranular film at the grain boundary. Besides, the oxidation resistance of high entropy carbide powders is greatly improved compared with that of the mixed five carbide powders. This work clearly highlights the merits of highly porous high entropy (Zr1/5Hf1/5Nb1/5Ta1/5Ti1/5)C as an ultra-high temperature thermal insulation material.

Key words: High entropy UHTCs, High porosity, High strength, Low thermal conductivity, Oxidation resistance

Zhuojie Shao, Zhen Wu, Luchao Sun, Xianpeng Liang, Zhaoping Luo, Haikun Chen, Junning Li, Jingyang Wang. High entropy ultra-high temperature ceramic thermal insulator (Zr_1/5Hf_1/5Nb_1/5Ta_1/5Ti_1/5)C with controlled microstructure and outstanding properties[J]. J. Mater. Sci. Technol., 2022, 119: 190-199.

Figures/Tables 9

Fig. 1. (a) XRD patterns of mixed powders and sintered samples with different SiC contents; (b) Rietveld refinement pattern of sample with 2 wt.% SiC content.

Fig. 2. SEM images of large pores, cell wall and crystal grains for porous high entropy carbide samples: (a)-(c) for HEC-10, (d)-(f) for HEC-15 and (g)-(i) for HEC-20.

Fig. 3. XRT images of porous high entropy carbide: (a) large pores and (b) cell wall for HEC-20.

Fig. 4. SEM-EDS analysis of (Zr1/5Hf1/5Nb1/5Ta1/5Ti1/5)C: (a) SEM image, and (b)-(f) corresponding EDS mappings.

Fig. 5. STEM-EDS analysis of porous high entropy carbide sample: (a) HAADF image, (b) corresponding ABF image, (c) SAED pattern and (d)-(i) corresponding EDS mappings.

Fig. 6. (a) Compressive strength and thermal conductivity of samples with different porosities at room temperature; (b) thermal conductivity of samples with different porosities as a function of temperature.

Fig. 7. (a) BSE image of cell wall surface of HEC-10, (b)-(f) HAADF images of cross-section containing grain boundary, (g) STEM and corresponding EDS mappings of porous high entropy carbide near surface of sintering neck.

Fig. 8. (a) STEM and corresponding EDS mappings of HEC-10 at interface of matrix grains; (b) HRTEM of porous sample at grain boundary and (c) corresponding FFT image of grain A/grain B interface, (d) inverse FFT image of a selected pair of diffraction spots, while the insert shows selected pair of diffraction spots of grain A.

Fig. 9. (a) DSC curves of mixed powders and high entropy carbide powders with 0 wt.%, 0.6 wt.% and 2 wt.% SiC; (b) corresponding TG curves of mixed powders and high entropy carbide powders with SiC additive.

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