(TiZrHf)P2O7: An equimolar multicomponent or high entropy ceramic with good thermal stability and low thermal conductivity

doi:10.1016/j.jmst.2019.05.030

Abstract

Abstract:

ZrP₂O₇ is a promising material for high temperature insulating applications. However, decomposition above 1400 °C is the bottleneck that limiting its application at high temperatures. To improve the thermal stability, a novel multicomponent equimolar solid solution (TiZrHf)P₂O₇ was designed and successfully synthesized in this work inspired by high-entropy ceramic (HEC) concept. The as-synthesized (TiZrHf)P₂O₇ exhibits good thermal stability, which is not decomposed after heating at 1550 °C for 3 h. It also shows lower thermal conductivity (0.78 W m^-1 K^-1) compared to the constituting metal pyrophosphates TiP₂O₇, ZrP₂O₇ and HfP₂O₇. The combination of high thermal stability and low thermal conductivity renders (TiZrHf)P₂O₇ promising for high temperature thermal insulating applications.

Key words: Metal phosphates, (TiZrHf)P₂O₇, High-entropy ceramics, Thermal stability, Thermal conductivity

Zifan Zhao, Huimin Xiang, ZhiDai Fu, Zhijian Peng, Yanchun Zhou. (TiZrHf)P₂O₇: An equimolar multicomponent or high entropy ceramic with good thermal stability and low thermal conductivity[J]. J. Mater. Sci. Technol., 2019, 35(10): 2227-2231.

Figures/Tables 9

Fig. 1. Crystal structure of MP2O7 (M=Ti, Zr and Hf).

Fig. 2. Experimental XRD pattern of (TiZrHf)P2O7 powders synthesized at 1000 °C together with those of TiP2O7, ZrP2O7 and HfP2O7 powders.

Table 1 Diffraction angle 2θ and corresponding reflections (hkl) of MP2O7 (M=Ti, Zr, Hf) and (TiZrHf)P2O7 solid solution obtained from experimental XRD patterns.

Reflection (hkl)	2θ (degree)
Reflection (hkl)	(TiZrHf)P₂O₇	TiP₂O₇	ZrP₂O₇	HfP₂O₇
111	18.929	19.541	18.691	18.775
200	21.887	22.597	21.607	21.709
021	24.508	25.299	24.175	24.293
112	26.893	27.761	26.520	26.654
202	31.132	32.156	30.714	30.855
311	36.689	37.893	36.16	36.335
222	38.384	3.6469	37.832	38.009
302	40.002	41.340	39.431	39.625
400	44.595	45.245	43.945	44.159
410	46.033	47.607	45.379	45.582
114	47.49	49.069	46.763	46.981
313	48.852	50.507	48.123	48.342
024	50.211	51.908	49.450	49.681

Table 2 Refined structure parameters of MP2O7 (M= Ti, Zr, Hf) and (TiZrHf)P2O7 solid solution obtained from Rietveld refinement.

Compounds	TiP₂O₇	ZrP₂O₇	HfP₂O₇	(TiZrHf)P₂O₇
a (?)	7.8738	8.2528	8.2101	8.0979
M	(0.5, 0.5, 0.5)	(0.5, 0.5, 0.5)	(0.5, 0.5, 0.5)	(0.5, 0.5, 0.5)
P	(0.1103, 0.1103, 0.1103)	(0.1054, 0.1054, 0.1054)	(0.1073, 0.1073, 0.1073)	(0.1054, 0.1054, 0.1054)
O1	(0.0565, 0.2770, 0.0877)	(0.0545, 0.2717, 0.0711)	(0.0543, 0.2738, 0.0714)	(0.0547, 0.2869, 0.0683)
O2	(0, 0, 0)	(0, 0, 0)	(0, 0, 0)	(0, 0, 0)

Fig. 3. XRD patterns of the (TiZrHf)P2O7 powders and ZrP2O7 powders after annealing at 1550 °C for 3 h.

Fig. 4. XRD pattern of bulk (TiZrHf)P2O7 solid solution sample.

Fig. 5. (a) Microstructure of the surface of sintered (TiZrHf)P2O7 solid solution compact. (b) Grain size distribution of sintered (TiZrHf)P2O7 solid solution compact.

Fig. 6. SEM image of the surface of bulk (TiZrHf)P2O7 solid solution and the element distributions in the observed area analyzed by EDS.

Table 3 Thermal properties and density of (TiZrHf)P2O7 together with those of single component pyrophosphates at room temperature.

Compounds	D_th (mm²/s)	C_p (J mol^-1 K^-1)	ρ (g/cm³)	κ (W m^-1 K^-1)
TiP₂O₇	0.53	155.86	2.89	1.08
ZrP₂O₇	0.50	162.00	3.01	0.92
HfP₂O₇	0.41	165.86	4.09	0.79
(TiZrHf)P₂O₇	0.43	151.32	3.35	0.78

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(TiZrHf)P₂O₇: An equimolar multicomponent or high entropy ceramic with good thermal stability and low thermal conductivity

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