Oxidation behaviors of (Hf0.25Zr0.25Ta0.25Nb0.25)C and (Hf0.25Zr0.25Ta0.25Nb0.25)C-SiC at 1300-1500 °C

doi:10.1016/j.jmst.2020.05.037

Abstract

Abstract:

In this work, high-entropy ceramics (Hf_0.25 Zr_0.25Ta_0.25Nb_0.25)C (HZTNC) and HZTNC doped with 20 vol% SiC (HZTNC-SiC) were fabricated by spark plasma sintering. Their oxidation behavior was investigated over the temperature range of 1300-1500 °C for up to 60 min. Both HZTNC and HZTNC-SiC exhibited good oxidation resistance, and their weight change as a function of oxidation time obeyed a parabolic law. Through XRD, microstructure observation, and elemental mapping analysis of the oxide layers, it was found that the formation of Nb₂Zr₆O₁₇, Hf₆Ta₂O₁₇, and (Ta, Nb)₂O₅ mixed-oxide layers effectively protected the matrix from further oxidation. Microcracks began to appear on the oxide layer of HZTNC at high temperatures after 60 min of oxidation. However, the addition of SiC in HZTNC suppressed these microcracks at high temperatures due to the active oxidation of SiC. Compared with the oxides formed on HZTNC, the additional formation of Hf(Zr)SiO₄ on HZTNC-SiC could further improve its oxidation resistance over HZTNC ceramics.

Key words: High-entropy carbide, Oxidation resistance, Oxidation mechanism

Haoxuan Wang, Shouye Wang, Yejie Cao, Wen Liu, Yiguang Wang. Oxidation behaviors of (Hf_0.25Zr_0.25Ta_0.25Nb_0.25)C and (Hf_0.25Zr_0.25Ta_0.25Nb_0.25)C-SiC at 1300-1500 °C[J]. J. Mater. Sci. Technol., 2021, 60: 147-155.

Figures/Tables 13

Fig. 1. XRD patterns of the as-received ceramics.

Fig. 2. SEM images showing the polished surface of HZTNC and HZTNC-SiC ceramics (a) HZTNC, (b) HZTNCSiC.

Fig. 3. SEM surface images of HZTNC and HZTNC-SiC ceramics after isothermal oxidation at different temperatures: (a) HZTNC, 1300 °C, (b) HZTNC-SiC, 1300 °C, (c) HZTNC, 1400 °C, (d) HZTNC-SiC, 1400 °C, (e) HZTNC, 1500 °C, (f) HZTNC-SiC, 1500 °C.

Fig. 4. (a-c) Square of the specific weight change as a function of oxidation time at 1300, 1400, and 1500 °C; (d) the relationship between lnkp and the reciprocal of temperature.

Table 1 Calculated parabolic rate constants and activation energies for HZTNC, HZTNC-SiC, HZTTNC [35], HZTTNC-SiC [31] and ZrB2-SiC [46] ceramics.

	kp, 1300 °C	kp, 1400 °C	kp, 1500 °C	Activation energy
	(mg²/cm⁴ h	(mg²/cm⁴ h	(mg²/cm⁴ h	(kJ/mol)
HZTNC	26.31	47.46	64.07	103
HZTNC-SiC	6.36	15.03	22.42	146
HZTTNC	53.90	81.76	152.10	134
HZTTNC-SiC	18.30	32.67	56.69	130
ZrB₂-SiC	11.81	-	38.91	212

Fig. 5. XRD patterns of oxidized HZTNC and HZTNC-SiC ceramics at different temperatures: (a) HZTNC, (b) HZTNC-SiC.

Fig. 6. Cross-sectional morphologies and EDX mapping for five constituting elements of the oxidized HZTNC ceramics at 1300 °C for different time: (a) HZTNC, 20 min, (b) HZTNC, 60 min.

Fig. 7. Cross-sectional morphologies and EDX mapping for five constituting elements of the oxidized HZTNCSiC ceramics at 1300 °C for different time: (a) HZTNC-SiC, 20 min, (b) HZTNC-SiC, 60 min.

Fig. 8. Cross-sectional morphologies and EDX mapping for five constituting elements of the oxidized HZTNC ceramics at 1400 °C for different time: (a) HZTNC, 20 min, (b) HZTNC, 60 min.

Fig. 9. Cross-sectional morphologies and EDX mapping for five constituting elements of the oxidized HZTNCSiC ceramics at 1400 °C for different time: (a) HZTNC-SiC, 20 min, (b) HZTNC-SiC, 60 min.

Fig. 10. Cross-sectional morphologies and EDX mapping for five constituting elements of the oxidized HZTNC ceramics at 1500 °C for different time: (a) HZTNC, 20 min, (b) HZTNC, 60 min.

Fig. 11. Cross-sectional morphologies and EDX mapping for five constituting elements of the oxidized HZTNC-SiC ceramics at 1500 °C for different time: (a) HZTNC-SiC, 20 min, (b) HZTNC-SiC, 60 min. (*1 Hf(Zr)TiO4, Hf(Zr)SiO4, Nb(Ta)2O5 layer; 2 Hf-Zr-Ta-Nb-Si-O layer).

Fig. 12. Schematic oxide structure of HZTNC and HZTNC-SiC ceramics: (a) HZTNC, (b) HZTNC-SiC.

References 54

[1]	Z.F. Zhao, H. Chen, H.M. Xiang, F.Z. Dai, X.H. Wang, Z.J. Peng, Y.C. Zhou, J. Mater. Sci. Technol. 38(2020) 80-85. DOI URL
[2]	Y. Qin, J.X. Liu, F. Li, X.F. Wei, H.Z. Wu, G.J. Zhang, J. Adv. Ceram. 8(2019) 148-152. DOI URL
[3]	X.Q. Shen, J.X. Liu, F. Li, G.J. Zhang, Ceram. Int. 45(2019) 24508-24514. DOI URL
[4]	R.Z. Zhang, J. Reece, Michael , J. Mater. Chem. A. 7(2019) 22148-22162. DOI URL
[5]	H. Chen, H.M. Xiang, F.Z. Dai, J.C. Liu, Y.C. Zhou, J. Mater. Sci. Technol. 36(2020) 134-139. DOI URL
[6]	K. Wang, L. Chen, C.G. Xu, W. Zhang, Z.G. Liu, Y.J. Wang, J.H. Ouyang, X.H. Zhang, Y.D. Fu, Y. Zhou, J. Mater. Sci. Technol. 39(2020) 99-105. DOI URL
[7]	F. Li, W.C. Bao, S.K. Sun, L. Zhou, J.X. Liu, F.F. Xu, G.J. Zhang, Scripta Mater. 176(2020) 17-22. DOI URL
[8]	X.Q. Shen, J.X. Liu, F. Li, G.J. Zhang, Ceram. Int. 45(2019) 24508-24514.
[9]	F.Z. Dai, B. Wen, Y.J. Sun, H.M. Xiang, Y.C. Zhou, J. Mater. Sci. Technol. 43(2020) 168-174. DOI URL
[10]	A. Kumar, M. Gupta, Metals. Basel. 6 (9) (2016) 199.
[11]	X.L. Yan, L. Constantin, Y.F. Lu, J.F. Silvain, M. Nastasi, B. Cui, J. Am. Ceram. Soc. 101(2018) 4486-4491. DOI URL
[12]	D. Demirskyi, H. Borodianska, T.S. Suzuki, Y. Sakka, K. Yoshimi, O. Vasylkiv, Scripta. Mater. 164 (2019) 12-16.
[13]	H. Chen, B. Zhao, Z.F. Zhao, H.M. Xiang, F.Z. Dai, J.C. Liu, Y.C. Zhou, J. Mater. Sci. Technol. 47(2020) 216-222.
[14]	Z.F. Zhao, H. Chen, H.M. Xiang, F.Z. Dai, X.H. Wang, Z.J. Peng, Y.C. Zhou, J. Mater. Sci. Technol. 35(2019) 2892-2896.
[15]	F. Li, L. Zhou, J.X. Liu, Y.C. Liang, G.J. Zhang, J. Adv. Ceram. 8(2019) 576-582.
[16]	Z.F. Zhao, H. Chen, H.M. Xiang, F.Z. Dai, X.H. Wang, W. Xu, K. Sun, Z.J. Peng, Y.C. Zhou, J. Mater. Sci. Technol. 47(2020) 45-51.
[17]	C.M. Rost, E. Sachet, T. Borman, A. Moballegh, E.C. Dickey, D. Hou, J.L. Jones, S. Curtarolo, J.P. Maria, Nat. Commun. 6(2015) 8485. DOI URL PMID
[18]	X.F. Wei, Y. Qin, J.X. Liu, F. Li, Y.C. Liang, G.J. Zhang, J. Eur. Ceram. Soc. 40(2020) 935-941.
[19]	F. Li, Y. Lu, X.G. Wang, W.C. Bao, J.X. Liu, F.F. Xu, G.J. Zhang, Ceram. Int. 45(2019) 22437-22441.
[20]	X.F. Wei, J.X. Liu, F. Li, Y. Qin, Y.C. Liang, G.J. Zhang, J. Eur. Ceram. Soc. 39(2019) 2989-2994.
[21]	J. Dusza, P. svec, V. Girman, R. Sedlák, E.G. Castle, T. Csanádi, A. KovalCíková, M. J. Reece, J. Eur. Ceram. Soc. 38(2018) 4303-4307. DOI URL
[22]	J.Y. Zhou, J.Y. Zhang, F. Zhang, B. Niu, L.W. Lei, W.M. Wang, Ceram. Int. 44(2018) 22014-22018. DOI URL
[23]	S. Jiang, T. Hu, J. Gild, N. Zhou, J. Nie, M. Qin, T. Harrington, K. Vecchio, J. Luo, Scripta. Mater. 142(2018) 116-120. DOI URL
[24]	Z.F. Zhao, H. Chen, H.M. Xiang, F.Z. Dai, X.H. Wang, W. Xu, K. Sun, Z.J. Peng, Y.H. Zhou, J. Mater. Sci. Technol. 39(2020) 167-172. DOI URL
[25]	J. D˛abrowa, M. Stygar, A. Mikuła, A. Knapik, K. Mroczka, W. Tejchman, M. Danielewski, M. Martin, Mater. Lett. 216(2018) 32-36. DOI URL
[26]	J. Gild, K. Kaufmann, K. Vecchio, J. Luo, Scripta. Mater. 170(2019) 106-110. DOI URL
[27]	J. Yan, F. Liu, G. Ma, B. Gong, J. Zhu, X. Wang, W. Ao, C. Zhang, Y. Li, J. Li, Scripta Mater. 157(2018) 129-134. DOI URL
[28]	J. Gild, J. Braun, K. Kaufmann, E. Marin, T. Harrington, P. Hopkins, K. Vecchio, J. Luo, J. Mater, 5(2019) 337-343.
[29]	P. Sarker, T. Harrington, C. Toher, C. Oses, M. Samiee, J.P. Maria, D.W. Brenner, K.S. Vecchio, S. Curtarolo, Nat. Commun. 9(2018) 4980. DOI URL PMID
[30]	Sarkar , L. Velasco, D. Wang, Q.S. Wang, G. Talasila, L.D. Biasi, C. Kübe, T. Brezesinski, S.S. Bhattacharya, H. Hahn, B. Breitung, Nat.Commun. 9(2018) 3400.
[31]	H.X. Wang, Y.J. Cao, W. Liu, Y.G. Wang, Ceram. Int. 46(2020) 11160-11168. DOI URL
[32]	Y.Q. Tan, C. Chen, S.G. Li, X.C. Han, J.X. Xue, T. Liu, Z.S. Zhou, H.B. Zhang, J. Alloys Compd. 816(2020), 152523. DOI URL
[33]	K. Ren, Q.K. Wang, G. Shao, X.F. Zhao, Y.G. Wang, Scripta Mater. 178(2020) 382-386. DOI URL
[34]	Y. Dong, K. Ren, Y.H. Lu, Q.K. Wang, J. Liu, Y.G. Wang, J. Eur. Ceram. Soc. 39(2019) 2574-2579.
[35]	H.X. Wang, Y.J. Cao, W. Liu, Y.G. Wang, J. Eur. Ceram. Soc. (2020) (Submitted). URL PMID
[36]	Z. Teng, L.N. Zhu, Y.Q. Tan, S.F. Zeng, Y.H. Xia, Y.G. Wang, H.B. Zhang, J. Eur. Ceram. Soc. 40(2020) 1639-1643.
[37]	Z.F. Zhao, H.M. Xiang, F.Z. Dai, Z.J. Peng, Y.H. Zhou, J. Mater. Sci. Technol. 35(2019) 2647-2651.
[38]	R. Savino, M.D.S. Fumo, D. Paterna, M. Serpico, Aerosp. Sci. Technol. 9(2005) 151-160.
[39]	M. Le-Huu, H. Schmitt, S. Noll, M. Grieb, F.F. Schrey, A.J. Bauer, L. Frey, H. Ryssel, Microelectron. Reliab. 51(2011) 1346-1350.
[40]	K. Yueh, K.A. Terrani, J. Nucl. Mater. 448(2014) 380-388. DOI URL
[41]	Y. Katoh, L.L. Snead, I. Szlufarska, W.J. Weber, Curr. Opin. Solid State Mater. Sci. 16(2012) 143-152.
[42]	J. Gild, Y. Zhao, T. Harrington, S. Jiang, T. Hu, M.C. Quinn, W.M. Mellor, N. Zhou, K. Vecchio, J. Luo, Sci. Rep. 6(2016) 37946. DOI URL PMID
[43]	T.A. Parthasarathy, R.A. Rapp, M. Opeka, R.J. Kerans, Acta Mater. 55(2007) 5999-6010. DOI URL
[44]	P. Sarin, P.E. Driemeyer, R.P. Haggerty, D.K. Kim, J.L. Bell, Z.D. Apostolov, W.M. Kriven, J. Eur. Ceram. Soc. 30(2010) 2375-2386. DOI URL
[45]	S. Shimada, M. Inagaki, K. Matsui, J. Am. Ceram. Soc. 75(1992) 2671-2678. DOI URL
[46]	Y.G. Wang, B.S. Ma, L.L. Li, L.N. An, J. Am. Ceram. Soc. 95(2012) 374-378.
[47]	N. Li, P. Hu, X.H. Zhang, Y.Z. Liu, W.B. Han, Corros. Sci. 73(2013) 44-53.
[48]	Y.G. Wang, L. Luo, J. Sun, L.N. An, Corros. Sci. 74(2013) 154-158.
[49]	J.B. He, Y.G. Wang, L. Luo, L.N. An, J. Am. Ceram. Soc. 36(2016) 3769-3774.
[50]	B.E. Deal, A.S. Grove, J. Appl. Phys. 36(1965) 3770-3778.
[51]	N.S. Jacobson, B. Harder, D. Myers, J. Am. Ceram. Soc. 96(2013) 838-844.
[52]	H.E. Evans, Surf. Coat. Technol. 206(2011) 1512-1521. DOI URL
[53]	M. Martena, D. Botto, P. Fino, S. Sabbadini, M.M. Gola, C. Badini, Eng. Fail. Anal. 13(2006) 409-426. DOI URL
[54]	W.G. Fahrenholtz, J. Am. Ceram. Soc. 90(2007) 143-148.