Abstract
Pyroxene structure SrMg1–xLi2xGe2O6 (x = 0.025–0.1) ceramics were prepared by a solid-state reaction method. Examines the impact of Li substitution on the sintering behavior, lattice vibration, bond covalence, and dielectric properties of SrMgGe2O6 ceramics. SrMgGe2O6 (space group: C2/c) was detected by XRD. Li+ can enter the lattice to form SrMg1–xLi2xGe2O6 solid solution. Through Rietveld refinement results, the effect of the Li+ doped content on the microwave performances of SMLG ceramics was analyzed. SEM results showed that SrMg0.925Li0.15Ge2O6 ceramics had the best surface morphology at 950 °C, and exhibited excellent microwave dielectric properties of εr = 5.91, Qf = 36,985 GHz, τf = -59 ppm/ °C. The relationship between the Qf value of SMLG ceramics and the packing fraction, and the bond valence is discussed. Calculating MgO6 octahedral distortion and bond energy can explain the change in τf value. SMLG Ceramics is a strong candidate in the LTCC.
Similar content being viewed by others
Data availability
The authors confirm that the data supporting the findings of this study are available within the article.
References
F.F. Wu, D. Zhou, C. Du, B.B. Jin, C. Li, Z.M. Qi, S. Sun, T. Zhou, Q. Li, X.Q. Zhang, Design of a Sub-6 GHz dielectric resonator antenna with novel temperature-stabilized Sm1–xBixNbO4 (x = 0–0.15) microwave dielectric ceramics. ACS Appl. Mater. Interfaces 14(5), 7030–7038 (2022). https://doi.org/10.1021/acsami.1c24307
X. Ma, J. Du, X. Ji, L. Liu, H. Wu, H. Kimura, Y. Lu, Z. Yue, Influence of Sn4+ substitution for Zr4+ in Nd2Zr3(MoO4)9 and the impact on the crystal structure and microwave dielectric properties. J. Alloys Compd. (2022). https://doi.org/10.1016/j.jallcom.2021.162526
X. Wei, Y. He, K. Liu, P. Gao, X. Chen, X. Liu, H. Zhou, Sintering behavior, crystal structure, and microwave dielectric properties of a novel diopside SrMgGe2O6 ceramic and adjustment of its τf value. Ceram. Int. (2022). https://doi.org/10.1016/j.ceramint.2022.12.259
J. Bao, H. Li, X. Xu, W. Guo, Y. Chen, Y. Zhang, J. Du, H. Wu, G. Duan, Z. Yue, Crystal structure, Raman spectrum, bond characteristics, and terahertz time-domain spectrum of novel Na5Tm(MoO4)4 microwave dielectric ceramic with ultra-low sintering temperature and high quality factor. J. Alloys Compd. (2023). https://doi.org/10.1016/j.jallcom.2022.168652
Z. Fang, L.-X. Pang, D. Zhou, X.-L. Wang, S. Ren, W.-G. Liu, Low-loss and temperature stable (1–x)Ba3P2O8-xMg2B2O5 composite ceramics with low sintering temperature. J. Eur. Ceram. Soc. 43(5), 1972–1977 (2023). https://doi.org/10.1016/j.jeurceramsoc.2022.11.064
Y. He, X. Wei, Y. Wu, X. Chen, J. Yang, H. Zhou, Effects of packing fraction, lattice vibration, and bond valence on the microwave dielectric properties of low-ε garnet-type Ca3Sc2Ge3O12 ceramics. J. Solid State Chem. (2023). https://doi.org/10.1016/j.jssc.2023.123980
M. Yang, Y. Gao, Y. Zheng, X. Lu, H. Yang, X. Xu, P. Wu, Microwave dielectric properties of Ca1–xBaxMgSi2O6 ceramics. Ceram. Int. 48(7), 9407–9412 (2022). https://doi.org/10.1016/j.ceramint.2021.12.136
K. Du, C.-Z. Yin, J.-Q. Yang, W. Luo, X.-C. Wang, W.-Z. Lu, W. Lei, Crystal structure, far-infrared spectra, and microwave dielectric properties of bazirite-type BaZr(Si1–xGex)3O9 ceramics. Ceram. Int. 48(3), 3592–3599 (2022). https://doi.org/10.1016/j.ceramint.2021.10.139
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). https://doi.org/10.1016/j.ceramint.2020.11.123
P. Zhang, X. Tian, X. Fan, A novel BaMg1.98Zn0.02V2O8 ceramic with low dielectric loss and good temperature stability for low temperature co-fired ceramic technology. Ceram. Int. 48(24), 36186–36192 (2022). https://doi.org/10.1016/j.ceramint.2022.08.175
H. Wang, S. Li, K. Wang, X. Wang, H. Zhang, Y. Wu, X. Chen, H. Zhou, Sintering characteristic, structure, microwave dielectric properties, and compatibility with Ag of novel 3MgO-B2O3-xwt% BaCu(B2O5)-ywt% H3BO3 ceramics. J. Asian Ceram. (2022). https://doi.org/10.1080/21870764.2022.2053277
Q. Zhang, H. Su, H. Zhang, X. Tang, Bond, vibration and microwave dielectric characteristics of Zn1–x(Li0.5Bi0.5)xWO4 ceramics with low temperature sintering. J. Materiomics 8(2), 392–400 (2022). https://doi.org/10.1016/j.jmat.2021.08.003
H. Wang, S. Li, K. Wang, X. Chen, H. Zhou, Sintering behaviour and microwave dielectric properties of MgO-2B2O3-xwt%BaCu(B2O5)-ywt%H3BO3 ceramics. J. Adv. Ceram. 10(6), 1282–1290 (2021). https://doi.org/10.1007/s40145-021-0503-0
X. Zhong, Z. Xiao-Yun, H. Long, S. Tian-Xiu, D. Shi-Hua, H.A.N. Lin-Cai, ZBAS on the structure and dielectric property of BaAl2Si2O8. J. Inorg. Mater. (2018). https://doi.org/10.15541/jim20170509
C. Li, S. Ding, T. Song, Y. Zhang, H. Zhu, Structure and microwave dielectric properties of BaAl2−2xLi2xSi2O8–2x ceramics. Ceram. Int. 47(4), 4895–4904 (2021). https://doi.org/10.1016/j.ceramint.2020.10.062
Y. He, X. Wei, G. He, Y. Wu, X. Chen, H. Zhou, Sintering behavior, phase composition, microstructure, and dielectric properties of low-permittivity alkaline earth silicate Sr3MgSi2O8 ceramics. J. Mater. Sci. Mater. Electron. (2022). https://doi.org/10.1007/s10854-022-09310-6
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). https://doi.org/10.1021/acsami.0c18836
S.-Z. Hao, D. Zhou, F. Hussain, W.-F. Liu, J.-Z. Su, D.-W. Wang, Q.-P. Wang, Z.-M. Qi, C. Singh, S. Trukhanov, Structure, spectral analysis and microwave dielectric properties of novel x(NaBi)0.5MoO4-(1–x)Bi2/3MoO4 (x=0.2 similar to 0.8) ceramics with low sintering temperatures. J. Eur. Ceram. Soc. 40(10), 3569–3576 (2020). https://doi.org/10.1016/j.jeurceramsoc.2020.03.074
H. Li, C. Cai, Q. Xiang, B. Tang, S. Yu, J. Xiao, H. Luo, S. Zhang, Raman, complex chemical bond and structural studies of novel CaMg1–x(Mn1/2Zn1/2)xSi2O6 (x=0–0.1) ceramics. Ceram. Int. 45(45), 23157–23163 (2019). https://doi.org/10.1016/j.ceramint.2019.08.010
S.-Z. Hao, D. Zhou, F. Hussain, J.-Z. Su, W.-F. Liu, D.-W. Wang, Q.-P. Wang, Z.-M. Qi, Novel scheelite-type Ca0.55(Nd1–xBix)0.3MoO4 (0.2 ≤ x ≤ 0.95) microwave dielectric ceramics with low sintering temperature. J. Am. Ceram. Soc. 103(12), 7259–7266 (2020). https://doi.org/10.1111/jace.17378
F. Huang, H. Su, Y. Li, H. Zhang, X. Tang, Low-temperature sintering and microwave dielectric properties of CaMg1−xLi2xSi2O6 (x = 0–0.3) ceramics. J. Adv. Ceram. 9(4), 471–480 (2020). https://doi.org/10.1007/s40145-020-0390-9
S. Liu, B. Tang, M. Zhou, P. Zhao, Q. Xiang, X. Zhang, Z. Fang, S. Zhang, Microwave dielectric characteristics of high permittivity Ca0.35Li0.25Nd0.35Ti1–x(Zn1/3Ta2/3)xO3 ceramics (x = 0.00–0.12). Ceram. Int. 45(7), 8600–8606 (2019). https://doi.org/10.1016/j.ceramint.2019.01.179
W. Liu, R. Zuo, Low temperature fired Ln2Zr3(MoO4)9 (Ln=Sm, Nd) microwave dielectric ceramics. Ceram. Int. 43(18), 17229–17232 (2017). https://doi.org/10.1016/j.ceramint.2017.09.083
W. Fang, Y. Tang, J. Chen, J. Li, L. Fang, Relationship between the structure and microwave dielectric properties of garnet ceramics Ca3B2GeV2O12 (B = Mg, Mn). Ceram. Int. 48(3), 4318–4323 (2022). https://doi.org/10.1016/j.ceramint.2021.10.226
R.D. Shannon, Dielectric polarizabilities of ions in oxides and fluorides. J. Appl. Phys. 73(1), 348–366 (1993). https://doi.org/10.1063/1.353856
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 (2022). https://doi.org/10.1021/acs.chemmater.2c02663
W. Yu, J. Lv, F. Shi, K. Song, W. Lei, H. Zhou, Z.-M. Qi, J. Wang, Lattice vibrational characteristics, crystal structure, and dielectric properties of single-phase Sr(Mg1/2Mo1/2)O3 microwave dielectric ceramic. J. Mater. Sci.: Mater. Electron. 32(13), 17191–17199 (2021). https://doi.org/10.1007/s10854-021-06182-0
P. Zhang, H. Li, X. Chen, X. Zhang, H. Yang, C. Li, S. Zhang, Influence of Re-ions with different ionic radius in Ba12ReNb9O36 on crystal structure and microwave dielectric properties. J. Materiomics 8(1), 104–112 (2022). https://doi.org/10.1016/j.jmat.2021.05.001
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). https://doi.org/10.1007/s40145-021-0472-3
J. Li, Y. Tang, Z. Zhang, W. Fang, L. Ao, A. Yang, L. Liu, L. Fang, Two novel garnet Sr3B2Ge3O12 (B = Yb, Ho) microwave dielectric ceramics with low permittivity and high Q. J. Eur. Ceram. Soc. 41(2), 1317–1323 (2021). https://doi.org/10.1016/j.jeurceramsoc.2020.10.018
N.E. Brese, M. O’Keeffe, Bond-valence parameters for solids. Acta Cryst. 47, 192–197 (1991)
M.G. Mason, S.T. Lee, G. Apai, R.F. Davis, D.A. Shirley, A. Franciosi, J.H. Weaver, Particle-size-induced valence changes in samarium clusters. Phys. Rev. Lett. 47(10), 730–733 (1981). https://doi.org/10.1103/PhysRevLett.47.730
K. Liu, C. Liu, J. Li, L. Jin, H. Zhang, Relationship between structure and properties of microwave dielectric ceramic Li(1+x)2MgTi3O8 based on Li non-stoichiometry. J. Materiomics 9(2), 279–288 (2023). https://doi.org/10.1016/j.jmat.2022.10.006
C. Li, S. Ding, Y. Zhang, H. Zhu, T. Song, Effects of Ni2+ substitution on the crystal structure, bond valence, and microwave dielectric properties of BaAl2–2xNi2xSi2O8–x ceramics. J. Eur. Ceram. Soc. 41(4), 2610–2616 (2021). https://doi.org/10.1016/j.jeurceramsoc.2020.12.011
K. Cheng, C. Li, C. Yin, Y. Tang, Y. Sun, L. Fang, Effects of Sr2+ substitution on the crystal structure, Raman spectra, bond valence and microwave dielectric properties of Ba3–xSrx(VO4)2 solid solutions. J. Eur. Ceram. Soc. 39(13), 3738–3743 (2019). https://doi.org/10.1016/j.jeurceramsoc.2019.05.030
X. Yan, S. Ding, Y. Zhang, T. Song, L. Huang, X. Zhang, Structure and microwave dielectric properties of BaAl2−2x(CuSi)xSi2O8 ceramics. J. Mater. Sci. 31(3), 2591–2597 (2020). https://doi.org/10.1007/s10854-019-02798-5
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). https://doi.org/10.1039/c5dt02164b
W.-S. Xia, L.-X. Li, P.-F. Ning, Q.-W. Liao, W.K. Wong-Ng, Relationship between bond ionicity, lattice energy, and microwave dielectric properties of Zn(Ta1−xNbx)2O6 ceramics. J. Am. Ceram. Soc. 95(8), 2587–2592 (2012). https://doi.org/10.1111/j.1551-2916.2012.05231.x
X.-Q. Song, W. Lei, M.-Q. Xie, J. Li, X.-C. Wang, W.-Z. Lu, Sintering behaviour, lattice energy and microwave dielectric properties of melilite-type BaCo2Si2O7 ceramics. Mater. Res. Express. (2020). https://doi.org/10.1088/2053-1591/ab4f10
M. Xiao, S. He, J. Meng, P. Zhang, Bond ionicity, lattice energy, bond energy and the microwave dielectric properties of non-stoichiometric MgZrNb2+xO8+2.5x ceramics. Mater. Chem. Phys. (2020). https://doi.org/10.1016/j.matchemphys.2019.122412
Y. Zhang, X. Li, S. Ding, T. Song, Z. Yin, J. Dan, Crystal structure and microwave dielectric properties of Li-modified BaSi2O5 ceramics. J. Market. Res. 22, 2792–2805 (2023). https://doi.org/10.1016/j.jmrt.2022.12.132
Y. Zhang, X. Jiang, X. Guo, S. Ding, T. Song, High-Q×f value and temperature stable MgZrTa2O8 ceramics by Li heterovalent substitution. J. Alloys Compd. (2023). https://doi.org/10.1016/j.jallcom.2023.169043
Y. Lai, H. Su, G. Wang, X. Tang, X. Huang, X. Liang, H. Zhang, Y. Li, K. Huang, X.R. Wang, Low-temperature sintering of microwave ceramics with high Qf values through LiF addition. J. Am. Ceram. Soc. (2018). https://doi.org/10.1111/jace.16086
K. Du, C.Z. Yin, Y.B. Guo, X.C. Wang, W.Z. Lu, S.W. Ta, C.Y. Hu, W. Lei, The relationship between crystal structure and modified microwave dielectric properties of Ca3SnSi2–xGexO9 ceramics. J. Am. Ceram. Soc. 105(2), 1253–1264 (2021). https://doi.org/10.1111/jace.18174
J. Zhang, J. Li, Y. Sun, L. Fang, Densification, microwave dielectric properties and rattling effect of LiYbO2 ceramics with low ε and anomalous positive τ. J. Eur. Ceram. Soc. 42(16), 7455–7460 (2022). https://doi.org/10.1016/j.jeurceramsoc.2022.09.010
K. Xiao, C. Li, Y. Tang, Y. Tian, C. Yin, J. Chen, J. Li, L. Duan, H. Xiang, L. Fang, (1–x)Li4WO5-xLiF: a novel oxyfluoride system and their microwave dielectric properties. J. Alloys Compd. (2020). https://doi.org/10.1016/j.jallcom.2020.155320
T. Hong, Y. Hu, S. Bao, C. Luo, L. Ai, P. Jiang, J. Chen, Z. Duan, Low-temperature sintering and microwave dielectric properties of CaMoO4 ceramics. J. Electron. Mater. 48(2), 972–976 (2018). https://doi.org/10.1007/s11664-018-6807-3
Acknowledgements
This study was supported by the Natural Science Foundation of China (Nos. 61761015), the Natural Science Foundation of Guangxi (Nos. 2017GXNSFFA198011, 2018GXNSFFA050001), and the High-Level Innovation Team and Outstanding Scholar Program of Guangxi Institute.
Author information
Authors and Affiliations
Contributions
All authors contributed to the study conception and design. Material preparation, data collection and analysis were performed by YH, XW, WL, YW, JY, XC, and HZ. The first draft of the manuscript was written by YH and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.
Corresponding authors
Ethics declarations
Conflict of interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
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
He, Y., Wei, X., Luo, W. et al. Effects of Li substitution on the sintering behavior, lattice vibration, bond covalence and dielectric properties of SrMgGe2O6 ceramics. J Mater Sci: Mater Electron 34, 1435 (2023). https://doi.org/10.1007/s10854-023-10787-y
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s10854-023-10787-y