Medium-entropy (Me,Ti)0.1(Zr,Hf,Ce)0.9O2 (Me = Y and Ta): Promising thermal barrier materials for high-temperature thermal radiation shielding and CMAS blocking

doi:10.1016/j.jmst.2022.01.019

Abstract

Abstract:

With continuous enhancement of gas-turbine inlet temperature and rapid increase of radiant heat transfer, thermal barrier coating (TBC) materials with a combination of low thermal conductivity and good high-temperature thermal radiation shielding performance play vital roles in ensuring the durability of metallic blades. However, yttria-stabilized zirconia (YSZ), as the state-of-the-art TBC and current industry standard, is unable to meet such demands since it is almost translucent to high-temperature thermal radiation. Besides, poor corrosion resistance of YSZ to molten calcia-magnesia-alumina-silicates (CMAS) also impedes its application in sand, dust, or volcanic ash laden environments. In order to improve the high-temperature thermal radiation shielding performance and CMAS resistance of YSZ and further reduce its thermal conductivity, two medium-entropy (ME) oxide ceramics, ME (Y, Ti)_0.1(Zr, Hf, Ce)_0.9O₂ and ME (Ta, Ti)_0.1(Zr, Hf, Ce)_0.9O₂, were designed and prepared by pressureless sintering of binary powder compacts in this work. ME (Y, Ti)_0.1(Zr, Hf, Ce)_0.9O₂ presents cubic structure but a trace amount of secondary phase, while ME (Ta, Ti)_0.1(Zr, Hf, Ce)_0.9O₂ displays a combination of tetragonal phase (81.6 wt.%) and cubic phase (18.4 wt.%). Both ME (Y, Ti)_0.1(Zr, Hf, Ce)_0.9O₂ and ME (Ta, Ti)_0.1(Zr, Hf, Ce)_0.9O₂ possess better high-temperature thermal radiation shielding performance than YSZ. Especially, the high-temperature thermal radiation shielding performance of ME (Ta, Ti)_0.1(Zr, Hf, Ce)_0.9O₂ is superior to that of ME (Y, Ti)_0.1(Zr, Hf, Ce)_0.9O₂ due to its narrower band gap and correspondingly higher infrared absorbance (above 0.7) at the waveband of 1 to 5 μm. The two ME oxides also display significantly lower thermal conductivity than YSZ and close thermal expansion coefficients (TECs) to YSZ and Ni-based superalloys. In addition, the two ME oxides possess excellent CMAS resistance. After attack by molten CMAS at 1250 °C for 4 h, merely ∼2 μm thick penetration layer has been formed and the structure below the penetration layer is still intact. These results demonstrate that ME (Me, Ti)_0.1(Zr, Hf, Ce)_0.9O₂ (Me = Y and Ta), especially ME (Ta, Ti)_0.1(Zr, Hf, Ce)_0.9O₂, are promising thermal barrier materials for high-temperature thermal radiation shielding and CMAS blocking.

Key words: Medium-entropy ceramics, Thermal barrier coatings, Thermal radiation shielding, CMAS resistance, Infrared absorbance

Shuaihang Qiu, Huimin Xiang, Fu-Zhi Dai, Hailong Wang, Muzhang Huang, Chunlei Wan, Qing Meng, Jiangtao Li, Xiaohui Wang, Yanchun Zhou. Medium-entropy (Me,Ti)_0.1(Zr,Hf,Ce)_0.9O₂ (Me = Y and Ta): Promising thermal barrier materials for high-temperature thermal radiation shielding and CMAS blocking[J]. J. Mater. Sci. Technol., 2022, 123: 144-153.

Figures/Tables 11

Fig. 1. XRD patterns of ME (Y, Ti)0.1(Zr, Hf, Ce)0.9O2 and ME (Ta, Ti)0.1(Zr, Hf, Ce)0.9O2.

Table 1. Structural data of the cubic-phase ME (Y, Ti)0.1(Zr, Hf, Ce)0.9O2 and ME (Ta, Ti)0.1(Zr, Hf, Ce)0.9O2 and tetragonal-phase ME (Ta, Ti)0.1(Zr, Hf, Ce)0.9O2.

Material	a (Å)	b (Å)	c (Å)	α = β = γ (°)	z	Symmetry	Space group	Theoretical density (g/cm³)
(Y,Ti)_0.1(Zr,Hf,Ce)_0.9O₂	5.2198	—	—	90	4	Cubic	$Fm\bar{3}m$[225]	7.54
(Ta,Ti)_0.1(Zr,Hf,Ce)_0.9O₂	5.3466	—	—	90	4	Cubic	$Fm\bar{3}m$[225]	7.25
(Ta,Ti)_0.1(Zr,Hf,Ce)_0.9O₂	3.6237	3.6237	5.2340	90	2	Tetragonal	P4₂/nmc [137]	8.06

Table 2. VECs and crystal structures of ME (Y, Ti)0.1(Zr, Hf, Ce)0.9O2 and ME (Ta, Ti)0.1(Zr, Hf, Ce)0.9O2 together with those of Y0.17Zr0.83O2 and Y0.17Ta0.17Zr0.66O2.

Material	VEC	Crystal structure	Refs.
(Y,Ti)_0.1(Zr,Hf,Ce)_0.9O₂	5.317	Cubic	This work
(Ta,Ti)_0.1(Zr,Hf,Ce)_0.9O₂	5.350	Tetragonal (main)	This work
Y_0.17Zr_0.83O₂	5.277	Cubic	[51]
Y_0.17Ta_0.17Zr_0.66O₂	5.333	Tetragonal	[51]

Fig. 2. SEM micrographs of the polished surface and the corresponding EDS mapping of the as-sintered (a) ME (Y, Ti)0.1(Zr, Hf, Ce)0.9O2 and (b) ME (Ta, Ti)0.1(Zr, Hf, Ce)0.9O2.

Fig. 3. (a, b) UV-Vis spectra, (c, d) (αhν)2 versus hν (Tauc) plots, and (e, f) (αhν)0.5 versus hν (Tauc) plots of ME (Y, Ti)0.1(Zr, Hf, Ce)0.9O2 and ME (Ta, Ti)0.1(Zr, Hf, Ce)0.9O2.

Fig. 4. (a) Infrared absorption spectra in the range from 1 to 2.5 μm and (b) infrared emissivity at the wavelength of 2.5 to 14 μm of ME (Y, Ti)0.1(Zr, Hf, Ce)0.9O2 and ME (Ta, Ti)0.1(Zr, Hf, Ce)0.9O2 ceramics.

Fig. 5. Thermal conductivity versus temperature curves of ME (Y, Ti)0.1(Zr, Hf, Ce)0.9O2, ME (Ta, Ti)0.1(Zr, Hf, Ce)0.9O2 and YSZ ceramics.

Table 3. Atomic radii and masses of different elements in ME (Y, Ti)0.1(Zr, Hf, Ce)0.9O2 and ME (Ta, Ti)0.1(Zr, Hf, Ce)0.9O2.

Element	Atomic radius (Å)	Mass (g/mol)
Y	1.82	89
Ta	1.47	181
Ti	1.47	48
Zr	1.60	91
Hf	1.59	179
Ce	1.81	140

Fig. 6. Thermal expansion curves of ME (Y, Ti)0.1(Zr, Hf, Ce)0.9O2 and ME (Ta, Ti)0.1(Zr, Hf, Ce)0.9O2 ceramics measured from room temperature to 1673 K.

Fig. 7. SEM images of the interfaces between the CMAS and the two ME oxides after CMAS corrosion: (a) ME (Y, Ti)0.1(Zr, Hf, Ce)0.9O2 and (b) ME (Ta, Ti)0.1(Zr, Hf, Ce)0.9O2.

Fig. 8. Line distribution of elements at the interfaces between the CMAS and the two ME oxides after CMAS corrosion: (a) ME (Y, Ti)0.1(Zr, Hf, Ce)0.9O2 and (b) ME (Ta, Ti)0.1(Zr, Hf, Ce)0.9O2.

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Medium-entropy (Me,Ti)_0.1(Zr,Hf,Ce)_0.9O₂ (Me = Y and Ta): Promising thermal barrier materials for high-temperature thermal radiation shielding and CMAS blocking

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