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Research Article | Open Access

Crystal structure, chemical bond characteristics, infrared reflection spectrum, and microwave dielectric properties of Nd2(Zr1−xTix)3(MoO4)9 ceramics

Jian BAOa, Yuping ZHANGa, Hideo KIMURAa, Haitao WUa(), Zhenxing YUEb()
School of Environmental and Material Engineering, Yantai University, Yantai 264005, China
State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China
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Abstract

Microwave dielectric ceramics (MWDCs) with low dielectric constant and low dielectric loss are desired in contemporary society, where the communication frequency is developing to high frequency (sub-6G). Herein, Nd2(Zr1−xTix)3(MoO4)9 (NZ1−xTxM, x = 0.02–0.10) ceramics were prepared through a solid-phase process. According to X-ray diffraction (XRD) patterns, the ceramics could form a pure crystal structure with the R3¯c (167) space group. The internal parameters affecting the properties of the ceramics were calculated and analyzed by employing Clausius–Mossotti relationship, Shannon’s rule, and Phillips–van Vechten–Levine (P–V–L) theory. Furthermore, theoretical dielectric loss of the ceramics was measured and analyzed by a Fourier transform infrared (IR) radiation spectrometer. Notably, when x = 0.08 and sintered at 700 ℃, optimal microwave dielectric properties of the ceramics were obtained, including a dielectric constant (εr) = 10.94, Q·f = 82,525 GHz (at 9.62 GHz), and near-zero resonant frequency temperature coefficient (τf) = −12.99 ppm/℃. This study not only obtained an MWDC with excellent properties but also deeply analyzed the effects of Ti4+ on the microwave dielectric properties and chemical bond characteristics of Nd2Zr3(MoO4)9 (NZM), which laid a solid foundation for the development of rare-earth molybdate MWDC system.

Keywords

microwave dielectric ceramics (MWDCs)Nd2(Zr1−xTix)3(MoO4)9 (NZ1−xTxM)Phillips–van Vechten–Levine (P–V–L) theorytheoretical dielectric loss

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Journal of Advanced Ceramics
Volume 12 Issue 1,
January 2023
Pages 82-92
DOI: 10.26599/JAC.2023.9220668
Cite this article:
BAO J, ZHANG Y, KIMURA H, et al. Crystal structure, chemical bond characteristics, infrared reflection spectrum, and microwave dielectric properties of Nd2(Zr1−xTix)3(MoO4)9 ceramics. Journal of Advanced Ceramics, 2023, 12(1): 82-92. https://doi.org/10.26599/JAC.2023.9220668
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10.26599/JAC.2023.9220668.T001Microwave dielectric properties of Ln2Zr3(MoO4)9 ceramics

MaterialTemperature (℃)εrQ·f (GHz)τf (ppm/℃)Ref.
Eu2Zr3(MoO4)960010.7574,900−8.88[14]
Sm2Zr3(MoO4)987511.0074,012−45.30[15]
NZM85010.8058,942−40.90[15]
Pr2Zr3(MoO4)965010.7264,200−13.00[16]
La2Zr3(MoO4)977510.8050,628−38.80[17]
Gd2Zr3(MoO4)972510.7840,945−12.26[18]
Ce2Zr3(MoO4)957510.6919,062−1.29[19]
Ce2(Zr0.92Sn0.08)3(MoO4)970010.2272,390−7.54[20]
Ce2(Zr0.96(Co1/2W1/2)0.04)3(MoO4)97509.9580,803−9.10[21]
Nd2(Zr0.92Ti0.08)3(MoO4)9(NZ0.92T0.08M)70010.9482,525−12.99This work

10.26599/JAC.2023.9220668.T002Crystal lattice parameters and reliability factors of NZ1−xTxM (x = 0.02–0.10) ceramics sintered at optimal temperatures

x valueCrystal lattice parameterReliability fator
a and b (Å)c (Å)α and β (°)γ (°)Molar volume V (Å3)Rp (%)Rwp (%)
0.029.806358.5110901204872.8245.647.40
0.049.799558.4966901204864.7964.946.63
0.069.793258.5010901204858.9965.997.91
0.089.783558.4743901204847.1316.658.71
0.109.776758.5337901204845.3063.614.87

10.26599/JAC.2023.9220668.T003Results obtained from the fitting of IR reflectivity spectrum of NZ0.92T0.08M

Modeωoj (cm−1)ωpj (cm−1)γj (cm−1)Δεj
1158.44225.2929.322.020
2163.4645.957.620.079
3169.8266.9212.620.155
4197.0451.879.670.069
5214.9387.4116.930.165
6275.60192.1616.710.486
7291.36137.2616.100.222
8310.02122.9726.770.157
9336.2791.698.550.074
10354.9255.798.880.025
11402.21163.9723.310.166
12429.96178.1724.120.172
13450.2787.2227.390.038
14657.76116.2928.680.031
15700.35355.0224.840.257
16735.09452.2818.870.379
17773.70181.3717.590.055
18810.31244.9322.480.091
19872.04112.3611.420.017
20887.26377.448.780.181
21897.69155.4312.240.030
22915.4664.6314.970.005
23955.88170.9310.650.032
24968.3648.788.490.003
NZ0.92T0.08Mε∞ = 3.07ε0 = 7.98