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A series of high-k [(Na0.5Bi0.5)xBi1−x](WxV1−x)O4 (abbreviated as NBWV(x value)) solid solution ceramics with a scheelite-like structure are synthesized by a modified solid-state reaction method at the temperature range of 680–760 ℃. A monoclinic (0 ≤ x < 0.09) to tetragonal scheelite (0.09 ≤ x ≤ 1.0) structural phase transition is confirmed by X-ray diffraction (XRD), Raman, and infrared (IR) analyses. The effect of structural deformation and order–disorder caused by Na+/Bi3+/W6+ complex substitution on microwave dielectric properties is investigated in detail. The compositional series possess a wide range of variable relative permittivity (εr = 24.8–80) and temperature coefficient of resonant frequency (TCF value, −271.9–188.9 ppm/℃). The maximum permittivity of 80 and a high Q×f value of ~10,000 GHz are obtained near the phase boundary at x = 0.09. Furthermore, the temperature-stable dielectric ceramics sintered at 680 ℃ with excellent microwave dielectric properties of εr = 80.7, Q×f = 9400 GHz (at 4.1 GHz), and TCF value = −3.8 ppm/℃ are designed by mixing the components of x = 0.07 and 0.08. In summary, similar sinterability and structural compatibility of scheelite-like solid solution systems make it potential for low-temperature co-fired ceramic (LTCC) applications.


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Sintering characteristics, phase transitions, and microwave dielectric properties of low-firing [(Na0.5Bi0.5)xBi1−x](WxV1−x)O4 solid solution ceramics

Show Author's information Xian XueaXiaomeng LibChangli FubYan ZhangdJing Guob( )Hong Wangc( )
State Key Laboratory for Mechanical Behavior of Materials, Faculty of Electronic and Information Engineering, Xi’an Jiaotong University, Xi’an 710049, China
State Key Laboratory for Mechanical Behavior of Materials, School of Materials Science and Engineering, Xi’an Jiaotong University, Xi’an 710049, China
Department of Materials Science and Engineering & Shenzhen Engineering Research Center for Novel Electronic Information Materials and Devices, Southern University of Science and Technology, Shenzhen 518055, China
Department of Physiology and Pathophysiology, Shaanxi Engineering and Research Center of Vaccine, Key Laboratory of Environment and Genes Related to Diseases of Education Ministry of China, School of Basic Medical Sciences, Xi’an Jiaotong University, Xi’an 710061, China

Abstract

A series of high-k [(Na0.5Bi0.5)xBi1−x](WxV1−x)O4 (abbreviated as NBWV(x value)) solid solution ceramics with a scheelite-like structure are synthesized by a modified solid-state reaction method at the temperature range of 680–760 ℃. A monoclinic (0 ≤ x < 0.09) to tetragonal scheelite (0.09 ≤ x ≤ 1.0) structural phase transition is confirmed by X-ray diffraction (XRD), Raman, and infrared (IR) analyses. The effect of structural deformation and order–disorder caused by Na+/Bi3+/W6+ complex substitution on microwave dielectric properties is investigated in detail. The compositional series possess a wide range of variable relative permittivity (εr = 24.8–80) and temperature coefficient of resonant frequency (TCF value, −271.9–188.9 ppm/℃). The maximum permittivity of 80 and a high Q×f value of ~10,000 GHz are obtained near the phase boundary at x = 0.09. Furthermore, the temperature-stable dielectric ceramics sintered at 680 ℃ with excellent microwave dielectric properties of εr = 80.7, Q×f = 9400 GHz (at 4.1 GHz), and TCF value = −3.8 ppm/℃ are designed by mixing the components of x = 0.07 and 0.08. In summary, similar sinterability and structural compatibility of scheelite-like solid solution systems make it potential for low-temperature co-fired ceramic (LTCC) applications.

Keywords: microwave ceramics, dielectric behavior, structural phase transition, order–disorder phenomena, low sintering temperatures

References(53)

[1]
Sebastian MT, Ubic R, Jantunen H. Low-loss dielectric ceramic materials and their properties. Int Mater Rev 2015, 60: 392–412.
[2]
Khan RU, Khan I, Ali B, et al. Structural, dielectric, optical, and electrochemical performance of Li4Mo5O17 for ULTCC applications. Mater Res Bull 2023, 160: 112142.
[3]
Guo J, Baker AL, Guo HZ, et al. Cold sintering process: A new era for ceramic packaging and microwave device development. J Am Ceram Soc 2017, 100: 669–677.
[4]
Guo WJ, Ma ZY, Luo Y, et al. Structure, defects, and microwave dielectric properties of Al-doped and Al/Nd co-doped Ba4Nd9.33Ti18O54 ceramics. J Adv Ceram 2022, 11: 629–640.
[5]
Yan TN, Dong C, Zhao JW, et al. Lead-free borosilicate glass/fused quartz composites for LTCC applications. J Mater Sci Mater Electron 2022, 33: 15033–15038.
[6]
Xue X, Li XM, Guo J, et al. Structure–property relationships in temperature stable low firing Ag2Mo2O7–Ag0.5Bi0.5MoO4 microwave dielectric ceramics. J Eur Ceram Soc 2022, 42: 6527–6532.
[7]
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.
[8]
Bi K, Wang XY, Hao YN, et al. Wideband slot-coupled dielectric resonator-based filter. J Alloys Compd 2019, 785: 1264–1269.
[9]
Yang S, Li L, Chen XM. Temperature dependence of τf and its origin in MgTiO3–CaTiO3 microwave dielectric composites. J Eur Ceram Soc 2022, 42: 5718–5725.
[10]
Harrop PJ. Temperature coefficients of capacitance of solids. J Mater Sci 1969, 4: 370–374.
[11]
Xiu ZY, Mao MM, Lu ZL, et al. High-Qf value and temperature stable Zn2+–Mn4+ cooperated modified cordierite-based microwave and millimeter-wave dielectric ceramics. J Eur Ceram Soc 2022, 42: 5712–5717.
[12]
Zhang X, Fang ZX, Yang HY, et al. Lattice evolution, ordering transformation and microwave dielectric properties of rock-salt Li3+xMg2−2xNb1−xTi2xO6 solid-solution system: A newly developed pseudo ternary phase diagram. Acta Mater 2021, 206: 116636.
[13]
Hao JY, Guo J, Fu CL, et al. The effects of cold sintering parameters on the densification of Na2WO4 ceramics using Na2WO4·2H2O dry powders. J Am Ceram Soc 2022, 105: 5058–5068.
[14]
Wang X, Shi JZ, Zhu XL, et al. Improved microwave dielectric characteristics in CaHf1−xTixO3 ceramics. J Am Ceram Soc 2023, 106: 1823–1833.
[15]
Qin TY, Zhong CW, Qin Y, et al. The structure evolution and microwave dielectric properties of MgAl2−x(Mg0·5Ti0.5)xO4 solid solutions. Ceram Int 2020, 46: 19046–19051.
[16]
Li XM, Zhang Y, Guo J, et al. Nonstoichiometric microwave dielectric ceramics [(Na0.5−xBi0.5+x/3)0.5Ca0.5]MoO4 with low sintering temperatures. J Eur Ceram Soc 2021, 41: 7029–7034.
[17]
Valant M, Suvorov D. Chemical compatibility between silver electrodes and low-firing binary-oxide compounds: Conceptual study. J Am Ceram Soc 2000, 83: 2721–2729.
[18]
Zhou D, Pang LX, Wang DW, et al. BiVO4 based high k microwave dielectric materials: A review. J Mater Chem C 2018, 6: 9290–9313.
[19]
Zhou D, Pang LX, Guo J, et al. Phase evolution, phase transition, and microwave dielectric properties of scheelite structured xBi(Fe1/3Mo2/3)O4–(1−x)BiVO4 (0.0 ≤ x ≤ 1.0) low temperature firing ceramics. J Mater Chem 2012, 22: 21412–21419.
[20]
Hanuza J, Mączka M, van der Maas JH. Polarized IR and Raman spectra of tetragonal NaBi(WO4)2, NaBi(MoO4)2 and LiBi(MoO4)2 single crystals with scheelite structure. J Mol Struct 1995, 348: 349–352.
[21]
Pang LX, Zhou D, Qi ZM, et al. Influence of W substitution on crystal structure, phase evolution and microwave dielectric properties of (Na0.5Bi0.5)MoO4 ceramics with low sintering temperature. Sci Rep 2017, 7: 3201.
[22]
Desu SB, O’Bryan HM. Microwave loss quality of BaZn13Ta2/3O3 ceramics. J Am Ceram Soc 1985, 68: 546–551.
[23]
Reaney IM, Wise PL, Qazi I, et al. Ordering and quality factor in 0.95BaZn1/3Ta2/3O3–0.05SrGa1/2Ta1/2O3 production resonators. J Eur Ceram Soc 2003, 23: 3021–3034.
[24]
Belous AG, Ovchar OV, Kramarenko AV, et al. Effect of nonstoichiometry on the structure and microwave dielectric properties of Ba(Co1/3Nb2/3)O3. Inorg Mater 2010, 46: 529–533.
[25]
Azough F, Freer R, Iddles D, et al. The effect of cation ordering and domain boundaries on low loss Ba(BI1/3BII2/3)O3 perovskite dielectrics revealed by high-angle annular dark-field scanning transmission electron microscopy (HAADF STEM). J Eur Ceram Soc 2014, 34: 2285–2297.
[26]
Bian JJ, Dong YF. New high Q microwave dielectric ceramics with rock salt structures: (1−x)Li2TiO3+xMgO system (0 ≤ x ≤ 0.5). J Eur Ceram Soc 2010, 30: 325–330.
[27]
Du MK, Li LX, Yu SH, et al. High-Q microwave ceramics of Li2TiO3 co-doped with magnesium and niobium. J Am Ceram Soc 2018, 101: 4066–4075.
[28]
Yuan XF, Zhang GQ, Wang H. A novel solid solution (K1−xNax)2Mo2O7 (0.0 ≤ x ≤ 0.3) ceramics with ultra-low sintering temperatures. J Eur Ceram Soc 2018, 38: 4967– 4971.
[29]
Xiong Y, Xie HY, Rao ZG, et al. Compositional modulation in ZnGa2O4 via Zn2+/Ge4+ co-doping to simultaneously lower sintering temperature and improve microwave dielectric properties. J Adv Ceram 2021, 10: 1360–1370.
[30]
Kshetri YK, Chaudhary B, Kamiyama T, et al. Determination of ferroelastic phase transition temperature in BiVO4 by Raman spectroscopy. Mater Lett 2021, 291: 129519.
[31]
Sleight AW, Chen HY, Ferretti A, et al. Crystal growth and structure of BiVO4. Mater Res Bull 1979, 14: 1571–1581.
[32]
Shannon RD, Oswald RA, Parise JB, et al. Dielectric constants and crystal structures of CaYAlO4, CaNdAlO4, and SrLaAlO4, and deviations from the oxide additivity rule. J Solid State Chem 1992, 98: 90–98.
[33]
Frost RL, Henry DA, Weier ML, et al. Raman spectroscopy of three polymorphs of BiVO4: Clinobisvanite, dreyerite and pucherite, with comparisons to (VO4)3− bearing minerals: Namibite, pottsite and schumacherite. J Raman Spectrosc 2006, 37: 722–732.
[34]
Zhang P, Tian X, Fan XY. Synthesis, sintering and microwave dielectric properties of Zn-doped Li3Mg4NbO8 ceramics. J Alloys Compd 2022, 925: 166818.
[35]
Choi W, Kim KY, Moon MR, et al. Effects of Nd2O3 on the microwave dielectric properties of BiNbO4 ceramics. J Mater Res 1998, 13: 2945–2949.
[36]
Fröhlichs H. Theory of Dielectrics: Dielectric Constant and Dielectric Loss. Oxford, UK: Clarendon Press, 1949.
[37]
Freer R, Azough F. Microstructural engineering of microwave dielectric ceramics. J Eur Ceram Soc 2008, 28: 1433–1441.
[38]
Wu FF, Zhou D, Du C, et al. Temperature stable Sm(Nb1−xVx)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.
[39]
Wang DX, Dursun S, Gao LS, et al. Fabrication of bimorph lead zirconate titanate thick films on metal substrates via the cold sintering-assisted process. Acta Mater 2020, 195: 482–490.
[40]
Chen HT, Tang B, Zhong CW, et al. The dielectric constant and quality factor calculation of the microwave dielectric ceramic solid solutions. Ceram Int 2017, 43: 7383–7386.
[41]
Tamura H. Microwave dielectric losses caused by lattice defects. J Eur Ceram Soc 2006, 26: 1775–1780.
[42]
Zhou D, Qu WG, Randall CA, et al. Ferroelastic phase transition compositional dependence for solid-solution [(Li0.5Bi0.5)xBi1−x][MoxV1−x]O4 scheelite-structured microwave dielectric ceramics. Acta Mater 2011, 59: 1502–1509.
[43]
Xiang HC, Yao L, Chen JQ, et al. Microwave dielectric high-entropy ceramic Li(Gd0.2Ho0.2Er0.2Yb0.2Lu0.2)GeO4 with stable temperature coefficient for low-temperature cofired ceramic technologies. J Mater Sci Technol 2021, 93: 28–32.
[44]
Song XQ, Zou ZY, Lu WZ, et al. Crystal structure, lattice energy and microwave dielectric properties of melilite-type Ba1−xSrxCu2Si2O7 solid solutions. J Alloys Compd 2020, 835: 155340.
[45]
Pei CJ, Tan JJ, Li Y, et al. Effect of Sb-site nonstoichiometry on the structure and microwave dielectric properties of Li3Mg2Sb1−xO6 ceramics. J Adv Ceram 2020, 9: 588–594.
[46]
Liu LT, Chen YG, Feng ZB, et al. Crystal structure, infrared spectra, and microwave dielectric properties of the EuNbO4 ceramic. Ceram Int 2021, 47: 4321–4326.
[47]
Kim MH, Lim JB, Nahm S, et al. Low temperature sintering of BaCu(B2O5)-added BaO–RE2O3–TiO2 (RE = Sm, Nd) ceramics. J Eur Ceram Soc 2007, 27: 3033–3037.
[48]
Zhou D, Randall CA, Wang H, et al. Ultra-low firing high-k scheelite structures based on [(Li0.5Bi0.5)xBi1−x][MoxV1−x]O4 microwave dielectric ceramics. J Am Ceram Soc 2010, 93: 2147–2150.
[49]
Pang LX, Zhou D, Yao XG, et al. Phase transitions and microwave dielectric behaviors of the (Bi1−xLi0.5xY0.5x)(V1−xMox)O4 ceramics. J Am Ceram Soc 2023, 106: 3455–3461.
[50]
Wu FF, Zhou D, Xia S, et al. Low sintering temperature, temperature-stable scheelite structured Bi[V1−x(Fe1/3W2/3)x]O4 microwave dielectric ceramics. J Eur Ceram Soc 2022, 42: 5731–5737.
[51]
Wang YY, Lv JQ, Wang J, et al. Lattice vibrational characteristics, crystal structure and dielectric properties of Ba2MgWO6 microwave dielectric ceramic. Ceram Int 2021, 47: 17784–17788.
[52]
Mei HR, Zhang LB, Rao ZG, et al. Na2CaTi2Ge3O12: An anti-reductive garnet ceramic with high quality factor and chemical compatibility with Cu/Ag electrodes for low temperature co-fired application. J Alloys Compd 2022, 926: 166960.
[53]
Li XM, Xue X, Lin QY, et al. Cold sintered temperature stable xLi2MoO4–(1−x)(LiBi)0.5MoO4 microwave dielectric ceramics. J Eur Ceram Soc 2023, 43: 1477–1482.
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Publication history

Received: 16 January 2023
Revised: 06 March 2023
Accepted: 23 March 2023
Published: 09 May 2023
Issue date: June 2023

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© The Author(s) 2023.

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant Nos. 61631166004 and 51902245). Hong Wang acknowledged the support of Shenzhen Science and Technology Program (Nos. KQTD20180411143514543 and JSGGZD20220822095603006). The XRD, SEM, and Raman tests were done in Instrumental Analysis Center of Xi’an Jiaotong University. The IR spectra experiment was performed by using the U4 beamline station at National Synchrotron Radiation Laboratory. The authors would like to thank Zeming Qi, Chuansheng Hu, and Hengjie Liu (National Synchrotron Radiation Laboratory) for the IR measurements.

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