Abstract
Novel Ni4Mg6Ge3O16(NMG) ceramics intermediate between olivine and spinel were synthesized using solid-state reaction method. The phase evolution, crystal structure, microstructure, and dielectric properties were also systematically characterized. The NMG ceramics show the main rhombohedral phase Ni4Mg6Ge3O16 and a small amount of NiMgO2 second phase. When the sintering temperature was increased to 1475 °C, the second phase is significantly reduced, and the NMG ceramic impart great dielectric properties parameters of εr = 7.1, Q × f = 53,245 GHz, and τf = − 38.7 ppm/°C. Moreover, the 0.55NMG-0.45TiO2 ceramic can be obtained (εr =14.78, Q × f = 40,559 GHz, τf = − 2.49 ppm/°C) with high thermal stability, reflecting that it has the potential for 5G device application.
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References
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, Design of a high-efficiency and -gain antenna using novel low-loss, temperature-stable Li2Ti1-x(Cu1/3Nb2/3)xO3 microwave dielectric ceramics. ACS Appl. Mater. Interfaces. 13(1), 912–923 (2021)
X. Zhou, H. Zhou, X. Luan, S. Hu, K. Wang, X. Wang, S. He, S. Zhou, J. Shi, X. Chen, Structure and dielectric properties of novel series of 3CaO–RE2O3–2WO3 (RE = La, Nd and Sm) microwave ceramics and the adjustment of τf value. J. Mater. Sci.: Mater. Electron. 31(17), 14953–14960 (2020)
I. Bakaimi, X.L. He, S. Guerin, N.Z.I. Hashim, Q. Luo, I.M. Reaney, S. Gao, B.E. Hayden, C.H.K. De Groot, Combinatorial synthesis and screening of (Ba, Sr)(Ti, Mn)O, thin films for optimization of tunable co-planar waveguides. J. Mater. Chem. C. 6(23), 6222–6228 (2018)
X. Dong, C.L. Sun, H.Y. Yang, L.Y. Yang, S.R. Zhang, Influence of Mg2SiO4 addition on crystal structure and microwave properties of Mg2Al4Si5O18 ceramic system. J. Mater. Sci.-Mater. Electron. 29(20), 17967–17973 (2018)
X.C. Lu, Z.H. Du, B. Quan, W.J. Bian, H.K. Zhu, Q.T. Zhang, Structural dependence of the microwave dielectric properties of Cr3+-substituted ZnGa2O4 spinel ceramics: crystal distortion and vibration mode studies. J. Mater. Chem. C. 7(27), 8261–8268 (2019)
H.H. Guo, D. Zhou, C. Du, P.J. Wang, W.F. Liu, L.X. Pang, Q.P. Wang, J.Z. Su, C. Singh, S. Trukhanov, Temperature stable Li2Ti0.75(Mg1/3Nb2/3)(0.25)O3-based microwave dielectric ceramics with low sintering temperature and ultra -low dielectric loss for dielectric resonator antenna applications. J. Mater. Chem. C. 8(14), 4690–4700 (2020)
S.H. Lei, H.Q. Fan, X.H. Ren, J.W. Fang, L.T. Ma, Z.Y. Liu, Novel sintering and band gap engineering of ZnTiO3 ceramics with excellent microwave dielectric properties. J. Mater. Chem. C. 5(16), 4040–4047 (2017)
B.Y. Qu, H.L. Du, Z.T. Yang, Lead-free relaxor ferroelectric ceramics with high optical transparency and energy storage ability. J. Mater. Chem. C. 4(9), 1795–1803 (2016)
B.J. Jeong, M.R. Joung, S.H. Kweon, J.S. Kim, S. Nahm, J.W. Choi, S.J. Hwang, Effect of Bi2O3 doping on the sintering temperature and microwave dielectric properties of LiAlSiO4 ceramics. J. Am. Ceram. Soc. 95(6), 1811–1813 (2012)
C.Z. Yin, Y. Tang, J.Q. Chen, F.H. Li, Y.J. Huang, C.C. Li, X.R. Xing, L. Fang, Two low-permittivity melilite ceramics in the SrO-MO-GeO2 (M = Mg, Zn) system and their temperature stability through compositional modifications. J. Eur. Ceram. Soc. 40(4), 1186–1190 (2020)
S.H. Kweon, M.R. Joung, J.S. Kim, B.Y. Kim, S. Nahm, J.H. Paik, Y.S. Kim, T.H. Sung, Low temperature sintering and microwave dielectric properties of B2O3-added LiAlSiO4 ceramics. J. Am. Ceram. Soc. 94(7), 1995–1998 (2011)
P. Gogoi, P. Sharma, D. Pamu, Microwave and broadband dielectric properties of Ni substituted MgTiO3 ceramics. J. Mater. Sci.-Mater. Electron. 27(9), 9052–9060 (2016)
C.Z. Yin, Y. Tang, J.Q. Chen, C.C. Li, L. Fang, F.H. Li, Y.J. Huang, Phase evolution, far-infrared spectra, and ultralow loss microwave dielectric ceramic of Zn2Ge1+xO4+2x (−01 ≤ x ≤ 02). J. Mater. Sci. Mater. Electron. 30(17), 16651–16658 (2019)
D. Zhou, C.A. Randall, H. Wang, L.X. Pang, X. Yao, Microwave dielectric ceramics in Li2O-Bi2O3-MoO3 system with ultra-low sintering temperatures. J. Am. Ceram. Soc. 93(4), 1096–1100 (2010)
K. Cheng, C.C. Li, H.C. Xiang, Y.H. Sun, L.F. Li, YGeO4: novel low-permittivity microwave dielectric ceramics with intrinsic low sintering temperature. Mater. Lett. 228, 96–99 (2018)
A. Manan, Z. Ullah, A.S. Ahmad, A. Ullah, D.F. Khan, A. Hussain, M.U. Khan, Phase microstructure evaluation and microwave dielectric properties of (1–x)Mg0.95Ni0.05Ti0.98Zr0.02O3-xCa(0.6)La(0.8/3)TiO(3) ceramics. J. Adv. Ceram. 7(1), 72–78 (2018)
J.S. Wei, P. Liu, H.X. Lin, Z.H. Ying, P. Zheng, W.T. Su, K.X. Song, H.B. Qin, Crystal structure and microwave dielectric properties of CaTiO3 modified Mg2Al4Si5O18 cordierite ceramics. J. Alloy. Compd. 689, 81–86 (2016)
H.L. Pan, M.T. Liu, M.F. Li, F. Ling, H.T. Wu, Low temperature sintering and microwave dielectric properties of Li6Mg7Ti3O16 ceramics with LiF additive for LTCC applications. J. Mater. Sci.-Mater. Electron. 29(2), 999–1003 (2018)
H.L. Pan, H.T. Wu, Crystal structure, infrared spectra and microwave dielectric properties of new ultra low-loss Li6Mg7Ti3O16 ceramics. Ceram. Int. 43(16), 14484–14487 (2017)
G. Schileo, A. Dias, R.L. Moreira, T.J. Jackson, P.A. Smith, K.T.S. Chung, A. Feteira, Structure and microwave dielectric properties of low firing Bi2Te2W3O16 ceramics. J. Am. Ceram. Soc. 97(4), 1096–1102 (2014)
K.G. Wang, H.F. Zhou, X.B. Liu, W.D. Sun, X.L. Chen, A. Ruan, A lithium aluminium borate composite microwave dielectric ceramic with low permittivity, near-zero shrinkage, and low sintering temperature. J. Eur. Ceram. Soc. 39(4), 1122–1126 (2019)
X. Zhou, K. Wang, S. Hu, X. Luan, S. He, X. Wang, S. Zhou, X. Chen, H. Zhou, Preparation, structure and microwave dielectric properties of novel La2MgGeO6 ceramics with hexagonal structure and adjustment of its τ value. Ceram. Int. 47(6), 7783–7789 (2021)
A. Manan, S.U. Khan, I. Qazi, Influence of sintering temperature on secondary phases formation and microwave dielectric properties of Ca2Ce2Ti5O16 ceramics. Mater. Sci. 32(2), 297–300 (2014)
Y.Z. Hao, Q.L. Zhang, J. Zhang, C.R. Xin, H. Yang, Enhanced sintering characteristics and microwave dielectric properties of Li2TiO3 due to nano-size and nonstoichiometry effect. J. Mater. Chem. 22(45), 23885–23892 (2012)
D. Zhou, L.X. Pang, D.W. Wang, I.M. Reaney, BiVO4 based high k microwave dielectric materials: a review. J. Mater. ChemC. 6(35), 9290–9313 (2018)
H.C. Xiang, Y. Bai, C.C. Li, L. Fang, H. Jantunen, Structural, thermal and microwave dielectric properties of the novel microwave material Ba2TiGe2O8. Ceram. Int. 44(9), 10824–10828 (2018)
Z.J. Song, K.X. Song, B. Liu, P. Zheng, H.B. Bafrooei, W.T. Su, H.X. Lin, F. Shi, D.W. Wang, I.M. Reaney, Temperature-dependent dielectric and Raman spectra and microwave dielectric properties of gehlenite-type Ca2Al2SiO7 ceramics. Int. J. Appl. Ceram. Technol. 17(2), 771–777 (2020)
K.P. Surendran, P.V. Bijumon, P. Mohanan, M.T. Sebastian, (1–x)MgAl2O4-xTiO2 dielectrics for microwave and millimeter wave applications. Appl. Phys. A-Mater. Sci. Process. 81(4), 823–826 (2005)
J.Q. Chen, Y. Tang, C.Z. Yin, M.Y. Yu, H.C. Xiang, C.C. Li, X.R. Xing, L. Fang, Structure, microwave dielectric performance, and infrared reflectivity spectrum of olivine-type Mg2Ge0.98O4 ceramic. J. Am. Ceram. Soc. 103(3), 1789–1797 (2020)
J. Cao, X.D. Yu, X.J. Kuang, Q. Su, Phase relationships in the BaO-Ga2O3-Ta2O5 system and the structure of Ba6Ga21TaO40. Inorg. Chem. 51(14), 7788–7793 (2012)
X.C. Liu, J.P. Deng, Phase structure and dielectric property of the ZnNb2O6-(Mg0.3Zn0.7)TiO3 multiphase ceramics. J. Mater. Sci.-Mater. Electron. 23(2), 506–510 (2012)
Y. Guo, H. Ohsato, K.-I. Kakimoto, Characterization and dielectric behavior of willemite and TiO2-doped willemite ceramics at millimeter-wave frequency. J. Eur. Ceram. Soc. 26(10–11), 1827–1830 (2006)
Z.Y. Tan, K.X. Song, H.B. Bafrooei, B. Liu, J. Wu, J.M. Xu, H.X. Lin, D.W. Wang, The effects of TiO2 addition on microwave dielectric properties of Y3MgAl3SiO12 ceramic for 5G application. Ceram. Int. 46(10), 15665–15669 (2020)
I. Kagomiya, J. Sugihara, K. Kakimoto, H. Ohsato, Liquid phase deposition process to deposit TiO2 in the porous Mg2SiO4 ceramics. J. Ceram. Soc. Jpn. 118(1380), 731–734 (2010)
Funding
This work was supported by the Natural Science Foundation of China (Nos. 61761015 and 11664008) and the Natural Science Foundation of Guangxi (Nos. 2017GXNSFFA198011, 2018GXNSFFA050001, and 2017GXNSFDA198027) and High-Level Innovation Team and Outstanding Scholar Program of Guangxi Institutes.
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All authors contributed to the study conception and design. Material preparation, data collection, and analysis were performed by SZ and XW. The first draft of the manuscript was written by SZ, and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.
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Zhou, S., Wang, X., Chen, X. et al. Structure and dielectric properties of low-permittivity thermal-stable NiO–MgO–GeO2 system ceramics. J Mater Sci: Mater Electron 33, 13455–13461 (2022). https://doi.org/10.1007/s10854-022-08242-5
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DOI: https://doi.org/10.1007/s10854-022-08242-5