Abstract
In this work, spinel-structured (1-x)Mg2TiO4-xLi4/3Ti5/3O4 (0.15 ≤ x ≤ 0.9) ceramic samples were fabricated by a conventional solid-state method. The samples exhibited a disordered-to-ordered-to-disordered structural transition with an increase in the x value. The compositional dependence of microwave dielectric properties of the samples was discussed with respect to the chemical bond characteristics. The dielectric constant (εr) was proved to be affected by the molar volume molecular polarizability and average bond ionicity (Afi). The quality factor (Q × f) was mainly dependent on the defect (i.e., Ti3+ and oxygen vacancy) population in the samples. Moreover, the temperature coefficient of the resonance frequency (τf) was confirmed to be affected by the Ti–O bond energy. The optimal microwave dielectric properties (εr = 26.0, Q × f = 36,500 GHz, and τf = 2.4 ppm/ºC) were achieved at x = 0.75.
Similar content being viewed by others
Data availability
All data generated or analyzed during this study are included in this published article.
References
I.S. Ghosh, A. Hilgers, T. Schlenker, R. Porath, Ceramic microwave antennas for mobile applications. J. Eur. Ceram. Soc. 21(15), 2621–2628 (2001)
M.T. Sebastian, H. Jantunen, Low loss dielectric materials for LTCC applications: a review. Int. Mater. Rev. 53(2), 57–90 (2008)
A. Belous, O. Ovchar, D. Durilin, M.M. Krzmanc, M. Valant, D. Suvorov, High-Q Microwave Dielectric Materials Based on the Spinel Mg2TiO4. J. Am. Ceram. Soc. 89(11), 3441–3445 (2006)
C.-L. Huang, S.-S. Liu, Low-loss microwave dielectrics in the (Mg1−xZnx)2TiO4 ceramics. J. Am. Ceram. Soc. 91(10), 3428–3430 (2008)
C.-L. Huang, J.-Y. Chen, Low-Loss Microwave Dielectric Ceramics Using (Mg1−xMnx)2TiO4 (x=0.02–0.1) Solid Solution. J. Am. Ceram. Soc. 92(3), 675–678 (2009)
C.-L. Huang, J.-Y. Chen, High-Q Microwave Dielectrics in the (Mg1−xCox)2TiO4 Ceramics. J. Am. Ceram. Soc. 92(2), 379–383 (2009)
C.L. Huang, C.E. Ho, Microwave dielectric properties of (Mg1−xNix)2TiO4 (x=0.02-0.1) ceramics: microwave dielectric properties. Int. J. Appl. Ceram. Technol. 7, E163–E169 (2010)
S. Liu, H. Li, R. Xiang, P. Zhang, X. Chen, Q. Wen, H. Hu, Effect of substituting Al3+ for Ti4+ on the microwave dielectric performance of Mg2Ti1-xAl4/3xO4 (0.01≤x≤0.09) ceramics. Ceram. Int. 47(23), 33064–33069 (2021)
R. Xiang, H. Li, P. Zhang, X. Chen, H. Hu, Q. Wen, S. Liu, Crystal structure and microwave dielectric properties of Mg2Ti1-xGa4/3xO4 (0.05≤x≤0.13) ceramics. Ceram. Int. 47(6), 8447–8452 (2021)
H. Li, B. Tang, Y. Li, Z. Qing, H. Chen, S. Zhang, Relationships between Sn substitution for Ti and microwave dielectric properties of Mg2(Ti1−xSnx)O4 ceramics system. J. Mater. Sci. Mater. Electron. 26(1), 571–577 (2015)
S.H. Kim, E.S. Kim, Intrinsic factors affecting the microwave dielectric properties of Mg2Ti1−x(Mg1/3Sb2/3)O4 ceramics. Ceram. Int. 42(13), 15035–15040 (2016)
S.H. Kim, E.S. Kim, Structural characteristics and microwave dielectric properties of Mg2Ti1-x(Mg1/3B2/3)xO4 (B=Nb5+, Ta5+) ceramics. Int. J. Nanotechnol. 15, 578 (2018)
X. Yang, Y. Lai, Y. Zeng, F. Yang, F. Huang, B. Li, F. Wang, C. Wu, H. Su, Spinel-type solid solution ceramic MgAl2O4-Mg2TiO4 with excellent microwave dielectric properties. J. Alloys Compd. 898, 162905 (2022)
W. Lei, W.-Z. Lu, D. Liu, J.-H. Zhu, Phase evolution and microwave dielectric properties of (1–x)ZnAl2O4−xMg2TiO4 ceramics. J. Am. Ceram. Soc. 92(1), 105–109 (2009)
Z. Cheng, L. Gan, X. Chu, D. Wang, Z. Qi, J. Jiang, T. Zhang, Investigation of the microwave dielectric properties of the Li4x/3Zn2−2xTi1+2x/3O4 system by P-V–L theory and vibration spectroscopy. Ceram. Int. 47(24), 34695–34703 (2021)
L. Nong, X. Cao, C. Li, L. Liu, L. Fang, J. Khaliq, Influence of cation order on crystal structure and microwave dielectric properties in xLi4/3Ti5/3O4-(1–x)Mg2TiO4 (0.6≤x≤0.9) spinel solid solutions. J. Eur. Ceram. Soc. 41(15), 7683–7688 (2021)
H. Li, R. Xiang, X. Chen, H. Hua, S. Yu, B. Tang, G. Chen, S. Zhang, Intrinsic dielectric behavior of Mg2TiO4 spinel ceramic. Ceram. Int. 46(4), 4235–4239 (2020)
H. Li, P. Zhang, S. Yu, H. Yang, B. Tang, F. Li, S. Zhang, Structural dependence of microwave dielectric properties of spinel structured Mg2(Ti1-xSnx)O4 solid solutions: crystal structure refinement, Raman spectra study and complex chemical bond theory. Ceram. Int. 45(9), 11639–11647 (2019)
D.C. Dube, R. Zurmuhlen, A. Bell, N. Setter, W. Wersing, Dielectric measurements on high-Q ceramics in the microwave region. J. Am. Ceram. Soc. 80(5), 1095–1100 (2005)
S. Kumar, R. Kumar, B.H. Koo, H. Choi, D.U. Kim, C.G. Lee, Structural and electrical properties of Mg2TiO4. J. Ceram. Soc. Jpn. 117(1365), 689–692 (2009)
C. Liu, H. Zhang, H. Su, T. Zhou, J. Li, X. Chen, W. Miao, L. Xie, L. Jia, Low temperature sintering BBSZ glass modified Li2MgTi3O8 microwave dielectric ceramics. J. Alloys Compd. 646, 1139–1142 (2015)
N. Leonidova, R.F. Samigullina, V. Patrakeev, Structural aspects of lithium transfer in solid electrolytes Li2xZn2–3xTi1+xO4 (0.33≤x≤0.67). J. Struct. Chem. 45(2), 262–268 (2004)
X. Chu, L. Gan, Z. Cheng, J. Jiang, J. Wang, T. Zhang, Investigation on the bond characteristics and microwave dielectric properties of rock salt-structured Li2Mg0.5nTiO3+0.5n (n=1–8) ceramics based on the complex chemical bond theory. Mater. Today. Commun. 36, 106675 (2023)
F. Wu, D. Zhou, C. Du, D.-M. Xu, R.-T. Li, Z.-Q. Shi, M.A. Darwish, T. Zhou, H. Jantunen, Design and fabrication of a satellite communication dielectric resonator antenna with novel low loss and temperature-stabilized (Sm1–xCax) (Nb1–xMox)O4 (x=0.15–0.7) microwave ceramics. Chem. Mater. 35(1), 104–115 (2023)
F.-F. Wu, D. Zhou, C. Du, D. Xu, R.-T. Li, L. Zhang, F. Qiao, Z.-Q. Shi, M.A. Darwish, T. Zhou, H. Jantunen, I.M. Reaney, Design and fabrication of a C-band dielectric resonator antenna with novel temperature-stable Ce(Nb1–xVx)NbO4 (x=0–0.4) microwave ceramics. ACS Appl. Mater. Interfaces 14(43), 48897–48906 (2022)
J.A. Van Vechten, Quantum dielectric theory of electronegativity in covalent systems. I. Electronic Dielectric Constant. Phys. Rev. 182(3), 891–905 (1969)
J.C. Phillips, Dielectric definition of electronegativity. Phys. Rev. Lett. 20(11), 550–553 (1968)
B.F. Levine, Bond susceptibilities and ionicities in complex crystal structures. J. Chem. Phys. 59(3), 1463–1486 (1973)
H. Yang, S. Zhang, H. Yang, E. Li, Usage of P-V–L bond theory in studying the structural/property regulation of microwave dielectric ceramics: a review. Inorg. Chem. Front. 7(23), 4711–4753 (2020)
S.S. Batsanov, Dielectric methods of studying the chemical bond and the concept of electronegativity. Russ. Chem. Rev. 51(7), 684–697 (1982)
M.T. Sebastian, R. Ubic, H. Jantunen, Low-loss dielectric ceramic materials and their properties. Int. Mater. Rev. 60(7), 392–412 (2015)
S. Takahashi, H. Ogawa, A. Kan, Electronic states and cation distributions of MgAl2O4 and Mg0.4Al2.4O4 microwave dielectric ceramics. J. Eur. Ceram. Soc. 38(2), 593–598 (2018)
X. Zhou, L. Liu, J. Sun, N. Zhang, H. Sun, H. Wu, W. Tao, Effects of (Mg1/3Sb2/3)4+ substitution on the structure and microwave dielectric properties of Ce2Zr3(MoO4)9 ceramics. J. Adv. Ceram. 10(4), 778–789 (2021)
D. Liu, S. Zhang, Z. Wu, Lattice energy estimation for inorganic ionic crystals. Inorg. Chem. 42(7), 2465–2469 (2003)
L. Li, Y. Li, J. Qiao, M. Du, Developing high-Q×f value MgNb2-xTaxO6(0≤x≤0.8) columbite ceramics and clarifying the impact mechanism of dielectric loss: crystal structure, Raman vibrations, microstructure, lattice defects, chemical bond characteristics, structural parameters, and microwave dielectric properties in-depth studies. J. Mater. Sci. Technol. 146, 186–199 (2023)
Z. Xiong, X. Zhang, B. Tang, C. Yang, Z. Fang, S. Zhang, Characterization of structure and properties in CaO-Nd2O3-TiO2 microwave dielectric ceramic modified by Al2O3. Mater Charact 176, 111108 (2021)
H. Borchert, Y. Borchert, V.V. Kaichev, I.P. Prosvirin, G.M. Alikina, A.I. Lukashevich, V.I. Zaikovskii, E.M. Moroz, E.A. Paukshtis, V.I. Bukhtiyarov, V.A. Sadykov, Nanostructured, Gd-doped ceria promoted by Pt or Pd: investigation of the electronic and surface structures and relations to chemical properties. J. Phys. Chem. B 109(43), 20077–20086 (2005)
X. Chu, L. Gan, S. Ren, J. Wang, Z. Ma, J. Jiang, T. Zhang, Low-loss and temperature-stable (1–x)Li2TiO3–xLi3Mg2NbO6 microwave dielectric ceramics. Ceram. Int. 46(6), 8413–8419 (2020)
E.M.C. Fortunato, L.M.N. Pereira, P.M.C. Barquinha, A.M. Botelho Do Rego, G. Gonçalves, A. Vilà, J.R. Morante, R.F.P. Martins, High mobility indium free amorphous oxide thin film transistors. Appl. Phys. Lett. 92(22), 222103 (2008)
Z. Cheng, L. Gan, Y. Liu, J. Jiang, T. Zhang, Microwave dielectric properties, low-temperature sintering mechanism, and defects behaviour of temperature stable (1–x)Li2Zn3Ti4O12-xSr3(VO4)2 ceramics. Ceram. Int. 48(16), 22789–22798 (2022)
P. Pyykkö, M. Atsumi, Molecular single-bond covalent radii for elements 1–118. Chemistry A European J. 15(1), 186–197 (2009)
Y.R. Luo, Comprehensive Handbook of Chemical Bond Energies (CRC Press, Boca Raton, 2007)
P. Zhang, Y. Zhao, W. Haitao, Bond ionicity, lattice energy, bond energy and microwave dielectric properties of ZnZr(Nb1−xAx)2O8 (A=Ta, Sb) ceramics. Dalton Trans. 44(38), 16684–16693 (2015)
Acknowledgements
This work was supported by the National Natural Science Foundation of China (Nos. 11774083 and 51902093).
Funding
This work was supported by the National Natural Science Foundation of China (Nos. 11774083 and 51902093).
Author information
Authors and Affiliations
Contributions
All authors contributed to the study conception and design. Material preparation, data collection and analysis were performed by BZ. The first draft of the manuscript was written by BZ and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.
Corresponding authors
Ethics declarations
Competing interests
The authors declare that they have no relevant financial or non-financial interests to disclose.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Zhang, B., Gan, L., Jiang, J. et al. Bond characteristics and microwave dielectric properties of temperature-stable (1-x)Mg2TiO4-xLi4/3Ti5/3O4 (0.15 ≤ x ≤ 0.9) spinel solid solutions. J Mater Sci: Mater Electron 35, 278 (2024). https://doi.org/10.1007/s10854-024-12056-y
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s10854-024-12056-y