Structure characteristics and microwave dielectric properties of Pr2(Zr1-xTix)3(MoO4)9 solid solution ceramic with a stable temperature coefficient

doi:10.1016/j.jmst.2021.10.051

Abstract

Abstract:

Pr₂(Zr_1-_xTi_x)₃(MoO₄)₉ (x = 0.1-1.0) ceramics were prepared via a conventional solid-state method, the dependence of crystal structure and bond characteristics on microwave dielectric properties was investigated systemically. The X-ray diffraction patterns indicated that the single-phase Pr₂Zr₃(MoO₄)₉ structure was formed in all the specimens. As the Ti⁴⁺ content increased, the lattice volume gradually decreased, which was ascribed to the fact that the ionic radius of Ti⁴⁺ was smaller than that of Zr⁴⁺. Notably, outstanding microwave dielectric properties with ε_r of 10.73-16.35, Q·f values of 80,696-18,726 GHz and minor τ_f values -14.1 - -2.6 ppm/ °C were achieved in Pr₂(Zr_1-_xTi_x)₃(MoO₄)₉ ceramics. The ε_r increased with the rising x values, which was associated with the increase of α/V_m values. The decreasing Q·f was affected by the decline of lattice energy of [Zr/TiO₆] octahedral. The τ_f value was dominated by [Zr/TiO₆] octahedral distortion, Mo-O bond energy, bond strength and B-site bond valence. Furthermore, infrared reflection spectra suggested that the properties were mainly caused by the absorption of phonon, and the dielectric loss could be further reduced by optimizing the experimental process.

Key words: Pr₂(Zr_1-xTi_x)₃(MoO₄)₉, Normalized bond length, Bond characteristics, Raman spectra

Huanrong Tian, Jinjie Zheng, Lintao Liu, Haitao Wu, Hideo Kimura, Yizhong Lu, Zhenxing Yue. Structure characteristics and microwave dielectric properties of Pr₂(Zr_1-_xTi_x)₃(MoO₄)₉ solid solution ceramic with a stable temperature coefficient[J]. J. Mater. Sci. Technol., 2022, 116: 121-129.

Figures/Tables 16

Fig. 1. Apparent density of the Pr2(Zr1-xTix)3(MoO4)9 ceramics sintered at different temperature; the sintering temperatures, corresponding to the maximum apparent density, as a function of x values are shown in the inset.

Fig. 2. The morphology of the Pr2(Zr1-xTix)3(MoO4)9 ceramics sintered at optimal temperature (a-j corresponding to 800 °C, 750 °C, 750 °C, 700 °C, 700 °C, 750 °C, 700 °C, 700 °C, 700 °C, 650 °C).

Fig. 3. XRD patterns of the Pr2(Zr1-xTix)3(MoO4)9 ceramics sintered at the optimal sintering temperatures (800 °C for x = 0.1, 750 °C for x = 0.2, 0.3, and 0.6, 700 °C for 0.4, 0.5, 0.7, 0.8, and 0.9, 650 °C for x = 1.0).

Fig. 4. The refinement patterns of the Pr2(Zr1-xTix)3(MoO4)9 ceramics sintered at optimal temperature (a-j corresponding to 800 °C, 750 °C, 750 °C, 700 °C, 700 °C, 750 °C, 700 °C, 700 °C, 700 °C, 650 °C).

Table 1. The lattice parameters and reliability factors of the Pr2(Zr1-xTix)3(MoO4)9 ceramics sintered at the optimal sintering temperatures.

x	Lattice parameter		Empty Cell	Empty Cell	Empty Cell	Reliability factors
x	a = b (Å)	c (Å)	α = β (°)	γ (°)	V_m (Å³)	R_p (%)	R_wp (%)
0.1	9.7904	58.6696	90	120	4870.22	7.14	9.14
0.2	9.7613	58.6646	90	120	4840.81	7.78	10.0
0.3	9.7421	58.6417	90	120	4819.92	8.97	11.5
0.4	9.6995	58.5572	90	120	4771.00	8.24	10.3
0.5	9.6952	58.4838	90	120	4760.85	8.13	10.2
0.6	9.6458	58.3466	90	120	4701.35	8.28	10.5
0.7	9.6098	58.1829	90	120	4653.26	7.69	9.69
0.8	9.5818	58.0186	90	120	4613.08	7.52	9.72
0.9	9.5487	57.8145	90	120	4565.14	8.98	11.6
1.0	9.5282	57.64019	90	120	4531.87	8.57	10.8

Fig. 5. Lattice parameters of the Pr2(Zr1-xTix)3(MoO4)9 ceramics as the function of the x values.

Fig. 6. The schematic diagram of Pr2(Zr1-xTix)3(MoO4)9 ceramics for (100) and (001) plane.

Fig. 7. (a) The average bond length and (b) the normalized bond length of different bonds as the function of the x values.

Fig. 8. (a) Dielectric constants (εr) of the Pr2(Zr1-xTix)3(MoO4)9 ceramics sintered at various temperatures, (b) the variation of εr and α/Vm as the function of the x values.

Fig. 9. (a) The Quality factors (Q·f) of the Pr2(Zr1-xTix)3(MoO4)9 ceramics sintered at different temperature, (b) the Q·f values and lattice energy (UZr/Ti-O) as the function of the x values.

Fig. 10. (a) The temperature coefficient of resonant frequency (τf), (b) [Zr/TiO4] octahedral distortion (Δ), (c) B-site bond valence (VB), (d) Mo-O bond strength (SMo-O), and (e) Mo-O bond energy (EMo-O) of the Pr2(Zr1-xTix)3(MoO4)9 ceramics as the function of x values.

Table 2. The character table of irreducible representations for the Pr2(Zr1-xTix)3(MoO4)9 ceramics.

D_3d(-3 m)	#	E	2C₃	3C₂	I	2S₆	3δ_d	Selection rules
A_1g	Γ₁⁺	1	1	1	1	1	1	α_xx+α_yy, α_zz
A_2g	Γ₂⁺	1	1	-1	1	1	-1	Rz
E_g	Γ₃⁺	2	-1	0	2	-1	0	(R_x, R_y), (α_xx-α_yy, α_xy), (α_xz, α_yz)
A_1u	Γ₁^-	1	1	1	-1	-1	-1	-
A_2u	Γ₂^-	1	1	-1	-1	-1	1	T_z
E_u	Γ₃^-	2	-1	0	-2	1	0	(T_x, T_y)

Table 3. Raman and IR vibrational modes of the Pr2(Zr1-xTix)3(MoO4)9 ceramics.

Atoms	Wyckoff positions	Symmetry	IR Active Modes						Raman Active Modes
Atoms	Wyckoff positions	Symmetry	A_1g	A_1u	A_2g	A_2u	E_u	E_g	A_1g	A_1u	A_2g	A_2u	E_u	E_g
Zr/Ti(1)	6b	S₆	-	-	-	1	2	-	-	-	-	-	-	-
Mo(1), O(1-6)	36f	C₁	-	-	-	3	6	-	3	-	-	-	-	6
Mo(2)	18e	C₂	-	-	-	2	3	-	1	-	-	-	-	3
Pr, Zr/Ti(2)	12c	C₃	-	-	-	1	2	-	1	-	-	-	-	2

Fig. 11. (a) The Raman spectra of Pr2(Zr1-xTix)3(MoO4)9 ceramics sintered at the optimal sintering temperatures (800 °C for x = 0.1, 750 °C for x = 0.2, 0.3, and 0.6, 700 °C for 0.4, 0.5, 0.7, 0.8, and 0.9, 650 °C for x = 1.0), (b) the measured and fitted Raman spectra of the Pr2(Zr1-xTix)3(MoO4)9 (x = 0.1, 1.0) ceramics, (c) the variation of Raman shift and τf with x from 0.1 to 1.0.

Fig. 12. (a) Measured and fitted infrared reflection spectra, (b) the real parts of the calculated and measured complex permittivity, and (c) the imaginary parts of the calculated and measured complex permittivity for the Pr2Ti3(MoO4)9 ceramics.

Table 4. Phonon parameters obtained from the fitting of the infrared reflectivity spectra of the Pr2Ti3(MoO4)9 ceramics.

ε_∞ = 3.06 ε = 10.65
j	ω_o_j	ω_p_j	γ_j	Δε_j
1	158.63	266.55	77.06	2.82
2	195.26	192.75	7.719	0.97
3	229.64	71.04	7.72	0.10
4	242.17	111.76	17.53	0.21
5	267.18	181.72	16.53	0.46
6	296.63	277.76	24.23	0.88
7	321.63	101.67	15.68	0.10
8	344.40	79.21	6.68	0.05
9	365.99	100.69	8.06	0.08
10	407.25	52.62	10.18	0.02
11	444.51	386.24	58.46	0.76
12	639.64	311.61	23.72	0.24
13	680.50	205.14	25.36	0.09
14	710.68	485.66	23.11	0.47
15	748.36	131.41	23.60	0.03
16	791.42	218.72	22.00	0.08
17	881.30	397.98	17.88	0.20
18	900.47	64.64	5.68	0.01
19	958.98	183.80	9.62	0.04

References 59

[1]	M.T. Sebastian, H. Jantunen, Int. Mater. Rev. 53 (2008) 57-90. DOI URL
[2]	J.M. Li, C.M. Zhang, H. Liu, T. Qiu, C.G. Fan, J. Adv. Ceram. 9 (2020) 558-566. DOI URL
[3]	D. Wang, S. Zhang, G. Wang, Y. Vardaxoglou, W. Whittow, D. Cadman, D. Zhou, K. Song, I.M. Reaney, Appl. Mater. Today 18 (2020) 100519.
[4]	Y. Li, B. Xu, S. Xia, P. Shi, J. Adv. Dielectr. 10 (2020) 2050027. DOI URL
[5]	C.J. Pei, J.J. Tan, Y. Li, G.G. Yao, Y.M. Jia, Z.Y. Ren, P. Liu, H.W. Zhang, J. Adv. Ceram. 9 (2020) 588-594. DOI URL
[6]	X.B. Ding, Y.J. Gu, Q. Li, B.H. Kim, Q.F. Wang, J.L. Huang, Ceram. Int. 46 (2020) 13225-13232. DOI URL
[7]	H.C. Yang, S.R. Zhang, H.Y. Yang, Q.Y. Wen, Q. Yang, L. Gui, Q. Zhao, E.Z. Li, J. Adv. Ceram. 10 (2021) 885-932. DOI URL
[8]	H.H. Guo, M.S. Fu, D. Zhou, C. Du, P.J. Wang, L.X. Pang, W.F. Liu, A.S.B. Sombra, J.Z. Su, ACS Appl. Mater. Int. 31 (2021) 912-923.
[9]	C.Z. Yin, Z.Z. Yu, L.L. Shu, L.J. Liu, Y. Chen, C.C. Li, J. Adv. Ceram. 10 (2021) 108-119. DOI URL
[10]	Z.Y. Tan, K.X. Song, H.B. Bafrooeia, B. Liu, J. Wu, J.M. Xu, H.X. Lin, D.W. Wang, Ceram. Int. 46 (2020) 15665-15669. DOI URL
[11]	F.Y. Huang, H. Su, Y.X. Li, H.W. Zhang, X.L. Tang, J. Adv. Ceram. 9 (2020) 471-480. DOI URL
[12]	C.Y. Cai, X.Q. Chen, H. Li, J. Xiao, C.W. Zhong, S.R. Zhang, Ceram. Int. 46 (2020) 27679-27685. DOI URL
[13]	M.T. Sebastian, H. Wang, H.L. Jantunen, Curr. Opin. Solid State Mater. 20 (2016) 151-170. DOI URL
[14]	J. Bao, J.L. Du, L.T. Liu, H.T. Wu, Y.Y. Zhou, Z.X. Yue, Ceram. Int. 48 (2022) 784-794. DOI URL
[15]	R. Peng, Y.X. Li, H. Su, Y.C. Lu, Y.R. Yun, L. Shi, B. Liao, J. Mater. Res. Technol. 9 (2020) 4994-5006. DOI URL
[16]	W.Q. Liu, R.Z. Zuo, Ceram. Int. 43 (2017) 17229-17232. DOI URL
[17]	J.J. Zheng, C.F. Xing, Y.K. Yang, S.X. Li, H.T. Wu, Z.H. Wang, J. Alloy Compd. 826 (2020) 153893. DOI URL
[18]	L. Shi, C. Liu, H.W. Zhang, J. Adv. Dielectr. 09 (2020) 1950049. DOI URL
[19]	J.J. Zheng, Y.H. Liu, B.J. Tao, Q. Zhang, H.T. Wu, X.Y. Zhang, Ceram. Int. 47 (2021) 5624-5630. DOI URL
[20]	Y.H. Zhang, J.J. Sun, N. Dai, Z.C. Wu, H.T. Wu, C.H. Yang, J. Eur. Ceram. Soc. 39 (2019) 1127-1131. DOI
[21]	B.J. Tao, C.F. Xing, W.F. Wang, H.T. Wu, Y.Y. Zhou, Ceram. Int. 45 (2019) 24675-24683. DOI
[22]	Y.H. Zhang, H.T. Wu, J. Am. Ceram. Soc. 102 (2019) 4092-4102. DOI URL
[23]	X. Zhou, L.T. Liu, J.J. Sun, N.K. Zhang, H.Z. Sun, H.T. Wu, W.H. Tao, J. Adv. Ceram. 10 (2021) 778-789. DOI URL
[24]	J.J. Zheng, Y.H. Liu, B.J. Tao, Q. Zhang, H.T. Wu, X.Y. Zhang, Ceram. Int. 47 (2021) 5624-5630. DOI URL
[25]	T. Tsunookaa, M. Androu, Y. Higashida, H. Sugiura, H. Ohsato, J. Eur. Ceram. Soc. 23 (2003) 2573-2578. DOI URL
[26]	A. Ullah, H.X. Liu, H. Hao, J. Iqbal, Z.H. Yao, M.H. Cao, J. Eur. Ceram. Soc. 37 (2017) 3045-3049. DOI URL
[27]	S.V. Zubkov, J. Adv. Dielectr. 11 (2021) 2160016. DOI URL
[28]	B.W. Hakki, P.D. Coleman, IEEE Trans. Microw. Theory 8 (1960) 402-410. DOI URL
[29]	W.E. Courtney, IEEE Trans. Microw. Theory 18 (1970) 476-485. DOI URL
[30]	N. Ichinose, T. Shimada, J. Eur. Ceram. Soc. 26 (2006) 1755-1759. DOI URL
[31]	J.I. Yang, S. Nahm, C.H. Choi, H.J. Lee, H.M. Park, J. Am. Ceram. Soc. 85 (2002) 165-168. DOI URL
[32]	H.C. Yang, S.R. Zhang, H.Y. Yang, Y. Yuan, E.Z. Li, Dalton Trans. 47 (2018) 15808-15815. DOI URL
[33]	R.D. Shannon, J. Appl. Phys. 73 (1993) 348-366. DOI URL
[34]	H.Y. Yang, S.R. Zhang, H.C. Yang, E.Z. Li, Inorg. Chem. Front. 7 (2020) 4711-4753. DOI URL
[35]	G. Wang, D.N. Zhang, X. Huang, Y.H. Rao, Y. Yang, G.W. Gan, Y.M. Lai, F. Xu, J. Li, Y.L. Liao, C. Liu, L.C. Jin, V.G. Harris, H.W. Zhang, J. Am. Ceram. Soc. 103 (2019) 214-223. DOI URL
[36]	X. Zhou, X.L. Ji, L.T. Liu, J.L. Du, H. Kimura, Y.Y. Zhou, Z.X. Yue, J.P. Wen, H.T. Wu, Ceram. Int. 48 (2022) 11056-11063. DOI URL
[37]	G. Wang, D.N. Zhang, J. Li, G.W. Gan, Y.H. Rao, X. Huang, Y. Yang, L. Shi, Y.L. Liao, C. Liu, L.C. Jin, H.W. Zhang, J. Am. Ceram. Soc. 103 (2020) 4321-4332. DOI URL
[38]	I.D. Brown, K.K. Wu, Acta Cryst. B 32 (1976) 1957-1959. DOI URL
[39]	J.X. Bi, C.F. Xing, C.H. Yang, H.T. Wu, J. Eur. Ceram. Soc. 38 (2018) 3840-3846. DOI URL
[40]	C. Feng, X. Zhou, B.J. Tao, H.T. Wu, S.F. Huang, J. Adv. Ceram. 11 (2022) 392-402. DOI URL
[41]	A.G. Cockbain, P.J. Harrop, Br. J. Appl. Phys. 1 (1968) 1109-1115.
[42]	P.J. Harrop, J. Mater. Sci. 4 (1969) 370-374. DOI URL
[43]	E.R. Kipkoech, F. Azough, R. Freer, J. Appl. Phys. 97 (2005) 064103. DOI URL
[44]	L.T. Nong, X.F. Cao, C.C. Li, L.J. Liu, L. Fang, J. Khaliq, J. Eur. Ceram. Soc. 41 (2021) 7683-7688. DOI URL
[45]	J. Dhanya, E.K. Suresh, R. Naveenraj, R. Ratheesh, J. Electron. Mater. 48 (2019) 4040-4049. DOI URL
[46]	E.J. Liang, H.L. Huo, J.P. Wang, M.J. Chao, J. Phys. Chem. C 112 (2008) 6577-6581. DOI URL
[47]	E.J. Liang, Y. Liang, Y. Zhao, J. Liu, Y.J. Jiang, J. Phys. Chem. A 112 (2008) 12582-12587. DOI PMID
[48]	J. Dhanya, P.V. Sarika, R. Naveenraj, E.K. Suresh, R. Ratheesh, Int. J. Appl. Ceram. Tec. 16 (2019) 1150-1158. DOI URL
[49]	H.C. Yang, S.R. Zhang, Y. Yuan, E.Z. Li, J. Am. Ceram. Soc. 103 (2019) 1131-1139. DOI URL
[50]	L. Shi, C. Liu, H.W. Zhang, R. Peng, G. Wang, X.L. Shi, X.Y. Wang, W.W. Wang, Mater. Chem. Phys. 250 (2020) 122954. DOI URL
[51]	V.V. Atuchin, V.G. Grossman, S.V. Adichtchev, N.V. Surovtsev, T.A. Gavrilova, B.G. Bazarov, Opt. Mater. 34 (2012) 812-816. DOI URL
[52]	R.F. Shen, B.H. Yuan, S.L. Li, X.H. Ge, J. Guo, E.J. Liang, Optik 165 (2018) 1-6. DOI URL
[53]	H. Li, X.Q. Chen, Q.Y. Xiang, B. Tang, J.W. Lu, Y.H. Zou, S.R. Zhang, Ceram. Int. 45 (2019) 14160-14166. DOI URL
[54]	K. Wakino, D.A. Sagala, H. Tamura, J. Am. Ceram. Soc. 69 (1986) 34-37. DOI URL
[55]	B. Liu, Y.H. Huang, H.B. Bafrooei, K.X. Song, L. Li, X.M. Chen, J. Eur. Ceram. Soc. 39 (2019) 4794-4799. DOI URL
[56]	L. Yi, X.Q. Liu, X.M. Chen, Int. J. Appl. Ceram. Technol. 12 (2015) E33-E40.
[57]	Y. Tang, M.Y. Xu, L. Duan, J.Q. Chen, C.C. Li, H.C. Xiang, L. Fang, J. Eur. Ceram. Soc. 39 (2019) 2354-2359. DOI URL
[58]	M.M. Mao, X.Q. Liu, X.M. Chen, J. Am. Ceram. Soc. 94 (2011) 2506-2511. DOI URL
[59]	Y. Tang, M.Y. Xu, L. Duan, J.Q. Chen, C.C. Li, H.C. Xiang, L. Fang, J. Eur. Ceram. Soc. 39 (2019) 2354-2359. DOI URL

Structure characteristics and microwave dielectric properties of Pr₂(Zr_1-_xTi_x)₃(MoO₄)₉ solid solution ceramic with a stable temperature coefficient

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