AI Chat Paper
Note: Please note that the following content is generated by AMiner AI. SciOpen does not take any responsibility related to this content.
{{lang === 'zh_CN' ? '文章概述' : 'Summary'}}
{{lang === 'en_US' ? '中' : 'Eng'}}
Chat more with AI
Powered by AMiner. Clicking this button will take you away from SciOpen.
Home Journal of Advanced Ceramics Article
PDF (7.1 MB)
Cite
EndNote(RIS) BibTeX
Collect
Submit Manuscript AI Chat Paper
Show Outline
Outline
Show full outline
Hide outline
Outline
Show full outline
Hide outline
Research Article | Open Access

Abnormal dielectric behavior of glaserite-type Ba3−xSrxMgSi2O8 solid solution

Jiaqing Yang1,2, Peng Lei1, Xiaoqiang Song2, Changzhi Yin2, Meng Zhang1,2, Weicheng Lei1,2, Yiyang Cai1,2, Mingfei Cheng1,2, Yaodong Liu1,2, Zihang Chen1,2, Yaqing Hu1,2, Wenzhong Lu1,2, Wen Lei1,2( )
School of Optical and Electronic Information, Key Lab of Functional Materials for Electronic Information (B) of MOE, Huazhong University of Science and Technology, Wuhan 430074, China
Wenzhou Key Laboratory of Microwave Communication Materials and Devices, Wenzhou Advanced Manufacturing Institute of HUST, Wenzhou 325035, China
Show Author Information

Graphical Abstract

Abstract

The temperature coefficient of the resonant frequency (τf) of low-permittivity (εr) microwave dielectric ceramics is required to be near 0 ppm/°C for practical application. However, owing to the polarization mechanism, τf of low-εr microwave dielectric ceramics is generally negative. Here, a novel microwave dielectric ceramic, Ba3−xSrxMgSi2O8, with an abnormal positive τf at the applied temperature is presented. In this study, Sr2+ with a relatively small ionic radius was introduced to replace Ba2+, and a single-phase solid solution was formed (x > 0.5). Ba3−xSrxMgSi2O8 ceramics were discussed in glaserite-type topology with space groups of P 3¯ for x ≤ 0.5, relatively high symmetry P 3¯m1 for 0.5 < x < 2.5, and C2 for x ≥ 2.5. The εr peaks as a function of temperature initially shift to low temperatures and then return to high temperatures through an ion substitution strategy. Notably, remarkable microwave dielectric properties for BaSr2MgSi2O8 were observed: εr ≈ 14.2, Q×f ≈ 38,900 GHz, and τf ≈ +117 ppm/°C, which are superior to those of other low-εr silicate ceramics with positive τf values. Density functional theory simulation calculations revealed that the preferential occupation of Sr2+ ions could decrease the intrinsic formation energy and improve the microwave dielectric properties by mitigating the ionic size mismatch within the crystal structure. The present research offers a strategy for discovering novel microwave dielectric ceramics with abnormal τf values, which could serve as τf regulators in practical applications because of their low cost and excellent microwave dielectric properties.

Keywords

microwave dielectric ceramicsabnormal dielectric behaviorion size mismatch[SiO4] tetrahedra tiltingphase transitiondensity functional theory (DFT)

References

[1]

Reaney IM, Iddles D. Microwave dielectric ceramics for resonators and filters in mobile phone networks. J Am Ceram Soc 2006, 89: 2063–2072.
Crossref Google Scholar
[2]

Kamutzki F, Schneider S, Barowski J, et al. Silicate dielectric ceramics for millimetre wave applications. J Eur Ceram Soc 2021, 41: 3879–3894.
Crossref Google Scholar
[3]

He GQ, Jiang Y, Song KX, et al. Ultrahigh- Q Sr1+ x Y2O4+ x ( x = 0.01–0.04) microwave dielectric ceramics for temperature-stable millimeter-wave dielectric resonator antennas. J Adv Ceram 2024, 13: 155–165.
Google Scholar
[4]

Hu X, Huang XJ, Chen YH, et al. Phase evolution and microwave dielectric properties of SrTiO3 added ZnAl2O4–Zn2SiO4–SiO2 ceramics. Ceram Int 2020, 46: 7050–7054.
Crossref Google Scholar
[5]

Yokoi A, Ogawa H, Kan A, et al. Microwave dielectric properties of Mg4Nb2O9–3.0wt% LiF ceramics prepared with CaTiO3 additions. J Eur Ceram Soc 2005, 25: 2871–2875.
Crossref Google Scholar
[6]

Surendran KP, Santha N, Mohanan P, et al. Temperature stable low loss ceramic dielectrics in (1− x)ZnAl2O4– xTiO2 system for microwave substrate applications. Eur Phys J B Condens Matter Complex Syst 2004, 41: 301–306.
Crossref Google Scholar
[7]
Li L, Yang S, Wu SY, et al. Nonlinear variation of resonant frequency with temperature and temperature-dependent τf in Al2O3–TiO2 microwave dielectric composites. 2021, 118 : 212902.
Crossref
[8]

Kolodiazhnyi T, Annino G, Spreitzer M, et al. Development of Al2O3–TiO2 composite ceramics for high-power millimeter-wave applications. Acta Mater 2009, 57: 3402–3409.
Crossref Google Scholar
[9]

Lei W, Zou ZY, Chen ZH, et al. Controllable τf value of barium silicate microwave dielectric ceramics with different Ba/Si ratios. J Am Ceram Soc 2018, 101: 25–30.
Crossref Google Scholar
[10]

Umemura R, Ogawa H, Yokoi A, et al. Low-temperature sintering-microwave dielectric property relations in Ba3(VO4)2 ceramic. J Alloys Compd 2006, 424: 388–393.
Crossref Google Scholar
[11]

Cheng K, Li CC, Yin CZ, et al. Effects of Sr2+ substitution on the crystal structure, Raman spectra, bond valence and microwave dielectric properties of Ba3− x Sr x (VO4)2 solid solutions. J Eur Ceram Soc 2019, 39: 3738–3743.
Crossref Google Scholar
[12]

Wu SP, Chen DF, Jiang C, et al. Synthesis of monoclinic CaSnSiO5 ceramics and their microwave dielectric properties. Mater Lett 2013, 91: 239–241.
Crossref Google Scholar
[13]
Tang Y, Zhang ZW, Li J, et al. A3Y2Ge3O12 (A = Ca, Mg): Two novel microwave dielectric ceramics with contrasting τf and Q×f. J Eur Ceram Soc 2020, 40 : 3989–3995.
Crossref
[14]

Wei JS, Xu ZH, Liu P, et al. Ba9Y2Si6O24: A new silicate dielectric ceramic for microwave communication application. Mater Lett 2016, 178: 144–146.
Crossref Google Scholar
[15]

Pang LX, Zhou D. Microwave dielectric properties of low-firing Li2 MO3 ( M = Ti, Zr, Sn) ceramics with B2O3–CuO addition. J Am Ceram Soc 2010, 93: 3614–3617.
Crossref Google Scholar
[16]

Ogawa H, Yokoi A, Umemura R, et al. Microwave dielectric properties of Mg3(VO4)2– xBa3(VO4)2 ceramics for LTCC with near zero temperature coefficient of resonant frequency. J Eur Ceram Soc 2007, 27: 3099–3104.
Crossref Google Scholar
[17]

Hao Z, Yue ZX, Meng SQ, et al. Low‐temperature sintering and microwave dielectric properties of Ba3(VO4)2–BaWO4 ceramic composites. J Am Ceram Soc 2008, 91: 3738–3741.
Crossref Google Scholar
[18]

Meng SQ, Yue ZX, Zhuang H, et al. Microwave dielectric properties of Ba3(VO4)2–Mg2SiO4 composite ceramics. J Am Ceram Soc 2009, 93: 359–361.
Google Scholar
[19]

Lv Y, Zuo RZ, Yue ZX. Structure and microwave dielectric properties of Ba3(VO4)2–Zn2- x SiO4− x ceramic composites. Mater Res Bull 2013, 48: 2011–2017.
Crossref Google Scholar
[20]

Dong ZW, Zheng Y, Cheng P, et al. Microwave dielectric properties of low-temperature sinterable Ba3(VO4)2–LiMgPO4 composite ceramics. Mater Lett 2014, 131: 151–153.
Crossref Google Scholar
[21]

Zhang J, Zuo RZ, Song J, et al. Low-loss and low-temperature firable Li2Mg3SnO6–Ba3(VO4)2 microwave dielectric ceramics for LTCC applications. Ceram Int 2018, 44: 2606–2610.
Crossref Google Scholar
[22]

Ding LF, Song MQ, Ma HT. Novel temperature-stable Mg2TiO4–Ba3(VO4)2 microwave dielectric ceramics for LTCC applications. Mater Chem Phys 2022, 289: 126488.
Crossref Google Scholar
[23]

Zhou T, Liu YH, Song KX, et al. New low- εr, temperature stable Mg3B2O6–Ba3(VO4)2 microwave composite ceramic for 5G application. J Am Ceram Soc 2021, 104: 3818–3822.
Crossref Google Scholar
[24]

Zhang ZW, Tang Y, Li J, et al. High- Q and near-zero τf composite Li2Mg2TiO5–Sr3(VO4)2 ceramics for low-temperature co-fired ceramic applications. Ceram Int 2020, 46: 8281–8286.
Crossref Google Scholar
[25]

Zhou HT, Xu ZN, Yan JY, et al. Temperature-stable BaAl2Si2O8–CaSnSiO5 microwave dielectric ceramics. Int J Appl Ceram Technol 2022, 19: 480–487.
Crossref Google Scholar
[26]

Lazoryak BI. Design of inorganic compounds with tetrahedral anions. Russ Chem Rev 1996, 65: 287–305.
Crossref Google Scholar
[27]

Rosica N, Vladislav K. Crystal chemistry of "glaserite" type compounds. Bulg Chem Commun 2013, 45: 418–426.
Google Scholar
[28]

Tsunooka T, Androu M, Higashida Y, et al. Effects of TiO2 on sinterability and dielectric properties of high- Q forsterite ceramics. J Eur Ceram Soc 2003, 23: 2573–2578.
Crossref Google Scholar
[29]

Song KX, Chen XM, Fan XC. Effects of Mg/Si ratio on microwave dielectric characteristics of forsterite ceramics. J Am Ceram Soc 2007, 90: 1808–1811.
Crossref Google Scholar
[30]

Gao Y, Zheng Y, Lu XP, et al. Synthesis and microwave dielectric properties of CaMg2Si3O9 ceramics. J Mater Sci Mater Electron 2020, 31: 21583–21590.
Crossref Google Scholar
[31]

Huang FY, Su H, Zhang Q, et al. Effect of Sr2+ substitution on the Raman spectrum, phase composition and microwave dielectric properties of CaMg1− x Sr x Si2O6 ceramics. Ceram Int 2022, 48: 3904–3911.
Crossref Google Scholar
[32]

Hameed I, Li L, Liu XQ, et al. Ultra low loss (Mg1– x Ca x )2SiO4 dielectric ceramics ( x = 0 to 0.15) for millimeter wave applications. J Am Ceram Soc 2022, 105: 2010–2019.
Crossref Google Scholar
[33]

Bafrooei HB, Liu B, Su WT, et al. Ca3MgSi2O8: Novel low-permittivity microwave dielectric ceramics for 5G application. Mater Lett 2020, 263: 127248.
Crossref Google Scholar
[34]

Zhang PC, Chen XQ, Chen GT, et al. Structural dependence of microwave dielectric properties of Ca3MgSi2O8 ceramics. J Mater Sci 2022, 57: 10039–10050.
Crossref Google Scholar
[35]

He YH, Wei XL, He GQ, et al. Sintering behavior, phase composition, microstructure, and dielectric properties of low-permittivity alkaline earth silicate Sr3MgSi2O8 ceramics. J Mater Sci Mater Electron 2022, 33: 26263–26275.
Crossref Google Scholar
[36]

Rodríguez-Carvajal J. Recent advances in magnetic structure determination by neutron powder diffraction. Phys B Condens Matter 1993, 192: 55–69.
Crossref Google Scholar
[37]
Yang Z, Lu Y, Zhao Q, et al. X-ray diffraction rietveld refinement and its application in cathode materials for lithium-ion batteries. J Inorg Mater 2023, 38 : 589.
Crossref
[38]

Courtney WE. Analysis and evaluation of a method of measuring the complex permittivity and permeability microwave insulators. IEEE Trans Microw Theory Tech 1970, 18: 476–485.
Crossref Google Scholar
[39]

Hakki BW, Coleman PD. A dielectric resonator method of measuring inductive capacities in the millimeter range. IEEE Trans Microw Theory Tech 1960, 8: 402–410.
Crossref Google Scholar
[40]

Kresse G, Furthmüller J. Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set. Comput Mater Sci 1996, 6: 15–50.
Crossref Google Scholar
[41]

Baroni S, de Gironcoli S, dal Corso A, et al. Phonons and related crystal properties from density-functional perturbation theory. Rev Mod Phys 2001, 73: 515–562.
Crossref Google Scholar
[42]

Kroumova E, Aroyo MI, Perez-Mato JM, et al. Bilbao crystallographic server: Useful databases and tools for phase-transition studies. Phase Transitions 2003, 76: 155–170.
Crossref Google Scholar
[43]
Diao CL, Wang CH, Luo NN, et al. First-principle calculation and assignment for vibrational spectra of Ba(Mg1/3Nb2/3)O3 microwave dielectric ceramic. 2014, 115 : 114103.
Crossref
[44]

Klaver TPC, Madsen GKH, Drautz R. A DFT study of formation energies of Fe–Zn–Al intermetallics and solutes. Intermetallics 2012, 31: 137–144.
Crossref Google Scholar
[45]

Kirklin S, Saal JE, Meredig B, et al. The open quantum materials database (OQMD): Assessing the accuracy of DFT formation energies. npj Comput Mater 2015, 1: 15010.
Crossref Google Scholar
[46]

Park SG, Magyari-Köpe B, Nishi Y. Electronic correlation effects in reduced rutile TiO2 within the LDA+U method. Phys Rev B 2010, 82: 115109.
Crossref Google Scholar
[47]
Yonezaki Y. (Ba,Sr)3MgSi2O8 structure change caused by Ba/Sr replacement. Powder Diffr 2015, 30 : 40–51.
Crossref
[48]

Park CH, Hong ST, Keszler DA. Superstructure of a phosphor material Ba3MgSi2O8 determined by neutron diffraction data. J Solid State Chem 2009, 182: 496–501.
Crossref Google Scholar
[49]
Yonezaki Y, Yanai R. X-ray induced electron defects in photochromic Ba3MgSi2O8:Eu3+ and isostructural K3Na(SO4)2. J Alloys Compd 2021, 876 : 160111.
Crossref
[50]

Yonezaki Y. Structural influence on photochromic behaviors of Eu2+-doped glaserite-type silicates. J Lumin 2018, 195: 408–412.
Crossref Google Scholar
[51]

Shannon RD. Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides. Acta Crystallogr Sect A 1976, 32: 751–767.
Crossref Google Scholar
[52]

Iwata T, Horie T, Fukuda K. Reinvestigation of crystal structure and structural disorder of Ba3MgSi2O8. Powder Diffr 2009, 24: 180–184.
Crossref Google Scholar
[53]

Fukuda K, Ito M, Iwata T. Crystal structure and structural disorder of (Ba0.65Ca0.35)2SiO4. J Solid State Chem 2007, 180: 2305–2309.
Crossref Google Scholar
[54]

Ye H, Li Y, Sun JL. Kinetic study on the anisotropic grain growth of elongated iron-containing mullite. Ceram Int 2019, 45: 12934–12941.
Crossref Google Scholar
[55]

Mouiya M, Tingaud D, Tamraoui Y, et al. Crystallography and anisotropy of crystals shape in dense aluminum titanate ceramics. J Eur Ceram Soc 2024, 44: 4761–4771.
Crossref Google Scholar
[56]

Bosman AJ, Havinga EE. Temperature dependence of dielectric constants of cubic ionic compounds. Phys Rev 1963, 129: 1593–1600.
Crossref Google Scholar
[57]

Wu FF, Zhou D, Du C, et al. A comprehensive study on crystal structure, phase compositions of the BiVO4–LaVO4 binary dielectric ceramic system and a typical design of dielectric resonator antenna for C-band applications. Appl Mater Today 2024, 38: 102222.
Crossref Google Scholar
[58]

Shannon RD. Dielectric polarizabilities of ions in oxides and fluorides. J Appl Phys 1993, 73: 348–366.
Crossref Google Scholar
[59]

Lyddane RH, Sachs RG, Teller E. On the polar vibrations of alkali halides. Phys Rev 1941, 59: 673–676.
Crossref Google Scholar
[60]

Zhou D, Pang LX, Qi ZM. Crystal structure and microwave dielectric behaviors of ultra-low-temperature fired x(Ag0.5Bi0.5)MoO4–(1– x)BiVO4 (0.0 ≤ x ≤ 1.0) solid solution with scheelite structure. Inorg Chem 2014, 53: 9222–9227.
Crossref Google Scholar
[61]

Zhou D, Pang LX, Wang H, et al. Phase transition, Raman spectra, infrared spectra, band gap and microwave dielectric properties of low temperature firing (Na0.5 x Bi1−0.5 x )(Mo x V1− x )O4 solid solution ceramics with scheelite structures. J Mater Chem 2011, 21: 18412–18420.
Crossref Google Scholar
[62]

Pang LX, Zhou D, Yao XG, et al. Phase transitions and microwave dielectric behaviors of the (Bi1– x Li0.5 x Y0.5 x )(V1– x Mo x )O4 ceramics. J Am Ceram Soc 2023, 106: 3455–3461.
Crossref Google Scholar
[63]

Kim ES, Chun BS, Freer R, et al. Effects of packing fraction and bond valence on microwave dielectric properties of A2+B6+O4 (A2+: Ca, Pb, Ba; B6+: Mo, W) ceramics. J Eur Ceram Soc 2010, 30: 1731–1736.
Crossref Google Scholar
[64]

Wu FF, Zhou D, Du C, et al. Temperature stable Sm(Nb1− x V x )O4(0.0 ≤ x ≤ 0.9) microwave dielectric ceramics with ultra-low dielectric loss for dielectric resonator antenna applications. J Mater Chem C 2021, 9: 9962–9971.
Crossref Google Scholar
[65]

Wang XY, Liu T, Cao ZK, et al. Lattice vibrational characteristics and structure-property relationships of Ca(Mg1/2W1/2)O3 microwave dielectric ceramics with different sintering temperatures. Ceram Int 2022, 48: 1415–1422.
Crossref Google Scholar
[66]

Yin CZ, Zou ZY, Cheng MF, et al. Microwave dielectric properties of CaB2O4–CaSiO3 system for LTCC applications. Crystals 2023, 13: 790.
Crossref Google Scholar
[67]

Xue X, Li XM, Fu CL, et al. Sintering characteristics, phase transitions, and microwave dielectric properties of low-firing [(Na0.5Bi0.5) x Bi1– x ](W x V1– x )O4 solid solution ceramics. J Adv Ceram 2023, 12: 1178–1188.
Crossref Google Scholar
[68]

Li JM, Wang ZX, Guo YF, et al. Influences of substituting of (Ni1/3Nb2/3)4+ for Ti4+ on the phase compositions, microstructures, and dielectric properties of Li2Zn[Ti1– x (Ni1/3Nb2/3) x ]3O8(0 ≤ x ≤ 0.3) microwave ceramics. J Adv Ceram 2023, 12: 760–777.
Crossref Google Scholar
[69]

Du K, Yin CZ, Guo YB, et al. Phase transition and permittivity stability against temperature of CaSn1− x Ti x GeO5 ceramics. J Eur Ceram Soc 2022, 42: 147–153.
Crossref Google Scholar
[70]

Su CX, Ao LY, Zhang ZW, et al. Crystal structure, Raman spectra and microwave dielectric properties of novel temperature-stable LiYbSiO4 ceramics. Ceram Int 2020, 46: 19996–20003.
Crossref Google Scholar
[71]

Cheng K, Tang Y, Xiang HC, et al. Two novel low permittivity microwave dielectric ceramics Li2Ti MO5 ( M = Ge, Si) with abnormally positive τf. J Eur Ceram Soc 2019, 39: 2680–2684.
Crossref Google Scholar
[72]

Song XQ, Du K, Zou ZY, et al. Temperature-stable BaAl2Si2O8–Ba5Si8O21-based low-permittivity microwave dielectric ceramics for LTCC applications. Ceram Int 2017, 43: 14453–14456.
Crossref Google Scholar
[73]

Manu KM, Karthik C, Leu LC, et al. Crystal structure and microwave dielectric properties of LiRE9(SiO4)6O2 ceramics (RE = La, Pr, Nd, Sm, Eu, Gd, and Er). J Am Ceram Soc 2013, 96: 1504–1511.
Crossref Google Scholar
[74]

Kweon SH, Joung MR, Kim JS, et al. Low temperature sintering and microwave dielectric properties of B2O3-added LiAlSiO4 ceramics. J Am Ceram Soc 2011, 94: 1995–1998.
Crossref Google Scholar
[75]

Thomas S, Sebastian MT. Microwave dielectric properties of SrRE4Si3O13 (RE=La, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Er, Tm, Yb, and Y) ceramics. J Am Ceram Soc 2009, 92: 2975–2981.
Crossref Google Scholar
[76]

Mao ZY, Chen JJ, Sun L, et al. Control of green emitting intermediate phases in (Ba,Sr)3MgSi2O8:Eu2+,Mn2+ phosphors for dual-bands or tri-bands emission. Mater Res Bull 2015, 70: 908–913.
Crossref Google Scholar
[77]

Song XQ, Xie MQ, Du K, et al. Synthesis, crystal structure and microwave dielectric properties of self-temperature stable Ba1− x Sr x CuSi2O6 ceramics for millimeter-wave communication. J Materiomics 2019, 5: 606–617.
Crossref Google Scholar
[78]

Khan N, Dollimore D, Alexander K, et al. The origin of the exothermic peak in the thermal decomposition of basic magnesium carbonate. Thermochim Acta 2001, 367: 321–333.
Crossref Google Scholar
[79]

Peng R, Lu YC, Zhang Q, et al. Amelioration of sintering and multi-frequency dielectric properties of Mg3B2O6: A mechanism study of nickel substitution using DFT calculation. J Adv Ceram 2021, 10: 1398–1407.
Crossref Google Scholar
Journal of Advanced Ceramics
Volume 14 Issue 2,
February 2025
Article number: 9221020
DOI: 10.26599/JAC.2024.9221020
Cite this article:
Yang J, Lei P, Song X, et al. Abnormal dielectric behavior of glaserite-type Ba3−xSrxMgSi2O8 solid solution. Journal of Advanced Ceramics, 2025, 14(2): 9221020. https://doi.org/10.26599/JAC.2024.9221020

542

Views

197

Downloads

0

Crossref

0

Web of Science

0

Scopus

0

CSCD

Altmetrics
Received: 30 September 2024
Revised: 24 November 2024
Accepted: 16 December 2024
Published: 07 January 2025
© The Author(s) 2025.

This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, http://creativecommons.org/licenses/by/4.0/).
Return