High-entropy Sm2B2O7 (B=Ti, Zr, Sn, Hf, Y, Yb, Nb, and Ta) oxides with highly disordered B-site cations for ultralow thermal conductivity

doi:10.1016/j.jmst.2021.12.038

Abstract

Abstract:

Materials with ultralow thermal conductivity and good thermal stability are of great interest in numerous applications such as energy storage and conversion devices, and thermal insulation components. In this work, a family of high-entropy Sm2B2O7 (B=Ti, Zr, Sn, Hf, Y, Yb, Nb, and Ta) oxides with highly disordered cations on the B-site has been synthesized by introducing large atomic-size mismatch, mass and charge disorder. Through tuning the composition, the high-entropy Sm2B2O7 oxides can be engineered from pyrochlore to fluorite structure, accompanied with an order-disorder transition. The pyrochlore Sm2(Nb0.2Sn0.2Ti0.2Y0.2Zr0.2)2O7 and fluorite Sm2(Nb0.2Ta0.2Y0.2Yb0.2Zr0.2)2O7 exhibit low thermal conductivities of 1.35 W·m-1·K-1 and 1.23 W·m-1·K-1, respectively, indicating their good thermal insulation. In addition, the high-entropy fluorite Sm2(Nb0.2Ta0.2Y0.2Yb0.2Zr0.2)2O7 also shows average thermal expansion coefficient of 10.2 × 10-6 °C-1 and high-temperature stability even after thermal exposure at 1600 °C in air for 30 h. These results indicate that the high-entropy Sm2B2O7 (B=Ti, Zr, Sn, Hf, Y, Yb, Nb, and Ta) can be promising candidates for thermal barrier coatings and thermally insulators.

Key words: High-entropy oxides, Atomic sizes mismatch, Mass and charge disorder, Thermal conductivity, Thermal barrier coatings materials

Liang Xu, Lei Su, Hongjie Wang, Hongfei Gao, Pengfei Guo, Min Niu, Kang Peng, Lei Zhuang, Zhiwei Dai. High-entropy Sm₂B₂O₇ (B=Ti, Zr, Sn, Hf, Y, Yb, Nb, and Ta) oxides with highly disordered B-site cations for ultralow thermal conductivity[J]. J. Mater. Sci. Technol., 2022, 119: 182-189.

Figures/Tables 10

Table 1. Compositions and molar ratio of raw materials of all specimens in this study.

Composition	Abbreviation	Molar ratio of raw materials
Sm₂(Hf_0.25Sn_0.25Ti_0.25Zr_0.25)₂O₇	S4TM	Sm₂O₃: HfO₂: SnO₂: TiO₂: ZrO₂=2: 1: 1: 1: 1
Sm₂(Hf_0.2Nb_0.2Sn_0.2Ti_0.2Zr_0.2)₂O₇	S5TM	Sm₂O₃: HfO₂: Nb₂O₅: SnO₂: TiO₂: ZrO₂=5: 2: 1: 2: 2
Sm₂(Nb_0.2Sn_0.2Ti_0.2Y_0.2Zr_0.2)₂O₇	Y-S5TM	Sm₂O₃: Nb₂O₅: SnO₂: TiO₂: Y₂O₃: ZrO₂=5: 1: 2: 2: 1: 2
Sm₂(Nb_0.2Ta_0.2Yb_0.2Y_0.2Zr_0.2)₂O₇	YY-S5TM	Sm₂O₃: Nb₂O₅: Ta₂O₅: Yb₂O₃: Y₂O₃: ZrO₂=5: 1: 1: 1:1: 2

Fig. 1. (a) Atomic model of (a) ideal 1/8 of a high-entropy pyrochlore unit cell and (b) a high-entropy fluorite unit cell; (c) XRD patterns of S4TM, S5TM, Y-S5TM and YY-S5TM samples prepared by calcined at 1500 °C for 20 h.

Table 2. Calculated lattice parameters, cations radii and ratio, and crystal structure of the high-entropy Sm2B2O7 oxides.

Composition	Abbreviation	Calculated lattice parameter (Å)	R_B-average	R_A/R_B	Structure type
Sm₂(Hf_0.25Sn_0.25Ti_0.25Zr_0.25)₂O₇	S4TM	10.453	0.681	1.584	Pyrochlore
Sm₂(Hf_0.2Nb_0.2Sn_0.2Ti_0.2Zr_0.2)₂O₇	S5TM	10.450	0.673	1.603	Pyrochlore
Sm₂(Nb_0.2Sn_0.2Ti_0.2Y_0.2Zr_0.2)₂O₇	Y-S5TM	10.464	0.711	1.518	Pyrochlore
Sm₂(Nb_0.2Ta_0.2Yb_0.2Y_0.2Zr_0.2)₂O₇	YY-S5TM	5.287	0.754	1.432	Fluorite

Fig. 2. Typical SEM micrographs and polished surface EDS scanning of the high-entropy Sm2B2O7 oxides, (a) Sm2(Hf0.25Sn0.25Ti0.25Zr0.25)2O7 (S4TM); (b) Sm2(Hf0.2Nb0.2Sn0.2Ti0.2Zr0.2)2O7 (S5TM); (c) Sm2(Nb0.2Sn0.2Ti0.2Y0.2Zr0.2)2O7 (Y-S5TM); (d) Sm2(Nb0.2Ta0.2Yb0.2Y0.2Zr0.2)2O7 (YY-S5TM).

Fig. 3. (a) Raman spectra of S4TM, S5TM, Y-S5TM and YY-S5TM samples; (b) the histogram the size disorder (δB), mass disorder (τB), and charge disorder (σB) of the high-entropy oxides (HEAO means high-entropy oxides with maximized disordered cations on the A-sites, (La/Y0.2Nd0.2Gd0.2Er0.2Lu0.2)2A2O7).

Fig. 4. (a) Thermal diffusivity and (b) thermal conductivity of the high-entropy Sm2B2O7 oxides, Sm2Zr2O7 [47], and YSZ [14,50]. Error bars represent the standard deviation.

Fig. 5. (a) Thermal expansion rates (dL/L0); (b) thermal expansion coefficients of the high-entropy Sm2B2O7 oxides

Table 3. Strength of ionic bond and thermal expansion coefficients of the high-entropy Sm2B2O7 oxides and Sm2Zr2O7.

Composition	Abbreviation	I_A-B	Thermal expansion coefficients (× 10^-6 °C^-1)
Sm₂Zr₂O₇	SZ	0.010	11.25
Sm₂(Hf_0.25Sn_0.25Ti_0.25Zr_0.25)₂O₇	S4TM	0.040	9.74
Sm₂(Hf_0.2Nb_0.2Sn_0.2Ti_0.2Zr_0.2)₂O₇	S5TM	0.042	9.49
Sm₂(Nb_0.2Sn_0.2Ti_0.2Y_0.2Zr_0.2)₂O₇	Y-S5TM	0.039	10.12
Sm₂(Nb_0.2Ta_0.2Yb_0.2Y_0.2Zr_0.2)₂O₇	YY-S5TM	0.012	10.18

Fig. 6. Thermal conductivities versus TECs for the high-entropy Sm2B2O7 oxides as well as other TBC materials [[56], [57], [58], [59], [60], [61], [62], [63], [64], [65], [66], [67], [68]].

Fig. 7. Thermal stability of the high-entropy Sm2B2O7 oxides: (a) TG-DSC analysis (air atmosphere, heating rate: 5 °C min-1); (b) phase stability after being treated at 1600 °C for 30 hours.

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High-entropy Sm₂B₂O₇ (B=Ti, Zr, Sn, Hf, Y, Yb, Nb, and Ta) oxides with highly disordered B-site cations for ultralow thermal conductivity

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