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In this study, low-temperature fired CaMg1-xLi2xSi2O6 microwave dielectric ceramics were prepared via the traditional solid-state reaction method. In this process, 0.4 wt% Li2CO3-B2O3-SiO2- CaCO3-Al2O3 (LBSCA) glass was added as a sintering aid. The results showed that ceramics consisted of CaMgSi2O6 as the main phase. The second phases were CaSiO3 always existing and Li2SiO3 occurring at substitution content x > 0.05. Li+ substitution effectively lowered sintering temperature due to 0.4 wt% LBSCA and contributed to grain densification, and the most homogeneous morphology could be observed at x = 0.05. The effects of relative density, the second phase, and ionic polarizability on dielectric constant (εr) were investigated. The quality factor (Q × f ) varied with packing fraction that concerned the second phase. Moreover, the temperature coefficient of the resonant frequency (τf) was influenced by MgO6 octahedral distortion and bond valence. Excellent dielectric properties of the CaMg1-xLi2xSi2O6 ceramic was exhibited at x = 0.05 with εr = 7.44, Q × f = 41,017 GHz (f = 15.1638 GHz), and τf = −59.3 ppm/℃ when sintered at 900 ℃. It had a good application prospect in the field of low-temperature co-fired ceramic (LTCC) substrate and devices.


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Low-temperature sintering and microwave dielectric properties of CaMg1-xLi2xSi2O6 (x = 0-0.3) ceramics

Show Author's information Fangyi HUANGaHua SUa,b( )Yuanxun LIa,bHuaiwu ZHANGaXiaoli TANGa
State Key Laboratory of Electronic Thin Films and Integrated Devices, University of Electronic Science and Technology of China, Chengdu 610054, China
Jiangxi Guo Chuang Industrial Park Development Co., Ltd., Ganzhou 341000, China

Abstract

In this study, low-temperature fired CaMg1-xLi2xSi2O6 microwave dielectric ceramics were prepared via the traditional solid-state reaction method. In this process, 0.4 wt% Li2CO3-B2O3-SiO2- CaCO3-Al2O3 (LBSCA) glass was added as a sintering aid. The results showed that ceramics consisted of CaMgSi2O6 as the main phase. The second phases were CaSiO3 always existing and Li2SiO3 occurring at substitution content x > 0.05. Li+ substitution effectively lowered sintering temperature due to 0.4 wt% LBSCA and contributed to grain densification, and the most homogeneous morphology could be observed at x = 0.05. The effects of relative density, the second phase, and ionic polarizability on dielectric constant (εr) were investigated. The quality factor (Q × f ) varied with packing fraction that concerned the second phase. Moreover, the temperature coefficient of the resonant frequency (τf) was influenced by MgO6 octahedral distortion and bond valence. Excellent dielectric properties of the CaMg1-xLi2xSi2O6 ceramic was exhibited at x = 0.05 with εr = 7.44, Q × f = 41,017 GHz (f = 15.1638 GHz), and τf = −59.3 ppm/℃ when sintered at 900 ℃. It had a good application prospect in the field of low-temperature co-fired ceramic (LTCC) substrate and devices.

Keywords:

low permittivity, low-temperature sintering, crystal structure, microwave dielectric properties
Received: 24 December 2019 Revised: 22 May 2020 Accepted: 22 May 2020 Published: 28 July 2020 Issue date: August 2020
References(44)
[1]
HI Hsiang, CC Chen, SY Yang. Microwave dielectric properties of Ca0.7Nd0.2TiO3 ceramic-filled CaO-B2O3-SiO2 glass for LTCC applications. J Adv Ceram 2019, 8: 345-351.
[2]
ZZ Weng, ZY Han, F Xiao, et al. Low temperature sintering and microwave dielectric properties of Zn1.8SiO3.8 ceramics with BaCu(B2O5) additive for LTCC applications. Ceram Int 2018, 44: 14145-14150.
[3]
P Zhang, KX Sun, L Liu, et al. A novel low loss and low temperature sintering Li3(Mg1-xCax)2NbO6 microwave dielectric ceramics by doping LiF additives. J Alloys Compd 2018, 765: 1209-1217.
[4]
EZ Li, HC Yang, HY Yang, et al. Effects of Li2O-B2O3-SiO2 glass on the low-temperature sintering of Zn0.15Nb0.3Ti0.55O2 ceramics. Ceram Int 2018, 44: 8072-8080.
[5]
XH Ma, SH Kweon, M Im, et al. Low-temperature sintering and microwave dielectric properties of B2O3- added ZnO-deficient Zn2GeO4 ceramics for advanced substrate application. J Eur Ceram Soc 2018, 38: 4682-4688.
[6]
HW Chen, H Su, HW Zhang, et al. Low-temperature sintering and microwave dielectric properties of (Zn1−xCox)2SiO4 ceramics. Ceram Int 2014, 40: 14655-14659.
[7]
XQ Song, K Du, J Li, et al. Low-fired fluoride microwave dielectric ceramics with low dielectric loss. Ceram Int 2019, 45: 279-286.
[8]
K Cheng, CC Li, HC Xiang, et al. LiYGeO4: Novel low- permittivity microwave dielectric ceramics with intrinsic low sintering temperature. Mater Lett 2018, 228: 96-99.
[9]
K Cheng, Y Tang, HC Xiang, et al. Two novel low permittivity microwave dielectric ceramics Li2TiMO5 (M = Ge, Si) with abnormally positive τf. J Eur Ceram Soc 2019, 39: 2680-2684.
[10]
WS Fang, K Cheng, HC Xiang, et al. Phase composition and microwave dielectric properties of low permittivity AGeO3 (A = Mg, Zn) ceramics. J Alloys Compd 2019, 799: 495-500.
[11]
CC Li, HC Xiang, MY Xu, et al. Li2AGeO4 (A = Zn, Mg): Two novel low-permittivity microwave dielectric ceramics with olivine structure. J Eur Ceram Soc 2018, 38: 1524-1528.
[12]
B Liu, CC Hu, YH Huang, et al. Crystal structure, infrared reflectivity spectra and microwave dielectric properties of CaAl2O4 ceramics with low permittivity. J Alloys Compd 2019, 791: 1033-1037.
[13]
XQ Song, K Du, J Li, et al. Crystal structures and microwave dielectric properties of novel low-permittivity Ba1-xSrxZnSi3O8 ceramics. Mater Res Bull 2019, 112: 178-181.
[14]
CZ Yin, CC Li, GJ Yang, et al. NaCa4V5O17: A low-firing microwave dielectric ceramic with low permittivity and chemical compatibility with silver for LTCC applications. J Eur Ceram Soc 2020, 40: 386-390.
[15]
CC Li, CZ Yin, JQ Chen, et al. Crystal structure and dielectric properties of germanate melilites Ba2MGe2O7 (M = Mg and Zn) with low permittivity. J Eur Ceram Soc 2018, 38: 5246-5251.
[16]
TY Qin, CW Zhong, Y Qin, et al. Low-temperature sintering mechanism and microwave dielectric properties of ZnAl2O4- LMZBS composites. J Alloys Compd 2019, 797: 744-753.
[17]
XQ Song, WZ Lu, XC Wang, et al. Sintering behaviour and microwave dielectric properties of BaAl2−2x(ZnSi)xSi2O8 ceramics. J Eur Ceram Soc 2018, 38: 1529-1534.
[18]
HP Sun, QL Zhang, H Yang, et al. (Ca1−xMgx)SiO3: A low-permittivity microwave dielectric ceramic system. Mater Sci Eng: B 2007, 138: 46-50.
[19]
H Li, XQ Chen, PC Zhang, et al. Influence of Mn2+ introduction on microwave dielectric properties of CaMgSi2O6 ceramic. Ceram Int 2019, 45: 24425-24430.
[20]
B Tang, QY Xiang, ZX Fang, et al. Influence of Cr3+ substitution for Mg2+ on the crystal structure and microwave dielectric properties of CaMg1-xCr2x/3Si2O6 ceramics. Ceram Int 2019, 45: 11484-11490.
[21]
YM Lai, H Su, G Wang, et al. Improved microwave dielectric properties of CaMgSi2O6 ceramics through CuO doping. J Alloys Compd 2019, 772: 40-48.
[22]
HP Wang, DH Li, QH Yang, et al. Sintering behavior and microwave dielectric properties of CaMgSi2O6 ceramics with Al2O3 addition. Mater Res Bull 2014, 54: 66-72.
[23]
HP Wang, SQ Xu, SY Zhai, et al. Effect of B2O3 additives on the sintering and dielectric behaviors of CaMgSi2O6 ceramics. J Mater Sci Technol 2010, 26: 351-354.
[24]
T Joseph, MT Sebastian, H Sreemoolanadhan, et al. Effect of glass addition on the microwave dielectric properties of CaMgSi2O6 ceramics. Int J Appl Ceram Technol 2009, 7: E98-E106.
[25]
SY Chang, HF Pai, CF Tseng, et al. Microwave dielectric properties of ultra-low temperature fired Li3BO3 ceramics. J Alloys Compd 2017, 698: 814-818.
[26]
D Thomas, MT Sebastian. Temperature-compensated LiMgPO4: A new glass-free low-temperature cofired ceramic. J Am Ceram Soc 2010, 93: 3828-3831
[27]
D Zhou, CA Randall, LX Pang, et al. Microwave dielectric properties of Li2WO4 ceramic with ultra-low sintering temperature. J Am Ceram Soc 2011, 94: 348-350.
[28]
XY Du, H Su, HW Zhang, et al. Effects of Li-ion substitution on the microwave dielectric properties of low- temperature sintered ceramics with nominal composition Li2xMg2−xSiO4. Ceram Int 2018, 44: 2300-2303.
[29]
XL Jing, XL Tang, WH Tang, et al. Effects of Zn2+ substitution on the sintering behaviour and dielectric properties of Li2Mg1−xZnxSiO4 ceramics. Appl Phys A 2019, 125: 415.
[30]
YZ Fan, ZY Zhou, RH Liang, et al. The effect of A-site nonstoichiometry on the microstructure, electric properties, and phase stability of NaNbO3 polycrystalline ceramics. J Eur Ceram Soc 2019, 39: 4712-4718.
[31]
EZ Li, X Yang, HC Yang, et al. Crystal structure, microwave dielectric properties and low temperature sintering of (Al0.5Nb0.5)4+ co-substitution for Ti4+ of LiNb0.6Ti0.5O3 ceramics. Ceram Int 2019, 45: 5418-5424.
[32]
ES Kim, BS Chun, R Freer, 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.
[33]
MJ Wu, YC Zhang, MQ Xiang. Synthesis, characterization and dielectric properties of a noveltemperature stable (1−x)CoTiNb2O8−xZnNb2O6 ceramic. J Adv Ceram 2019, 8: 228-237.
[34]
LH Ouyang, WQ Wang, HC Fan, et al. Sintering behavior and microwave performance of CaSiO3 ceramics doped with BaCu(B2O5) for LTCC applications. Ceram Int 2019, 45: 18937-18942.
[35]
YM Lai, XL Tang, HW Zhang, et al. Relationship between the structure and microwave dielectric properties of non-stoichiometric Li2+xSiO3 ceramics. Ceram Int 2017, 43: 2664-2669.
[36]
RD Shannon, GR Rossman. Dielectric constant of MgAl2O4 spinel and the oxide additivity rule. J Phys Chem Solids 1991, 52: 1055-1059.
[37]
RD Shannon. Dielectric polarizabilities of ions in oxides and fluorides. J Appl Phys 1993, 73: 348-366.
[38]
K Cheng, CC Li, CZ Yin, et al. 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 2019, 39: 3738-3743.
[39]
TA Yee, L Suescun, FA Rabuffetti. Bond valence parameters for alkali- and alkaline-earth-oxygen pairs: Derivation and application to metal−organic compounds. J Solid State Chem 2019, 270: 242-246.
[40]
NE Brese, M O'Keeffe. Bond-valence parameters for solids. Acta Crystallogr Sect B 1991, 47: 192-197
[41]
YM Lai, XL Tang, X Huang, et al. Phase composition, crystal structure and microwave dielectric properties of Mg2−xCuxSiO4 ceramics. J Eur Ceram Soc 2018, 38: 1508-1516.
[42]
YM Lai, H Su, G Wang, et al. Low-temperature sintering of microwave ceramics with high Qf values through LiF addition. J Am Ceram Soc 2019, 102: 1893-1903
[43]
WS Xia, LX Li, LJ Ji, et al. Phase evolution, bond valence and microwave characterization of (Zn1−xNix)Ta2O6 ceramics. Mater Lett 2012, 66: 296-298.
[44]
HS Park, KH Yoon, ES Kim. Effect of bond valence on microwave dielectric properties of complex perovskite ceramics. Mater Chem Phys 2003, 79: 181-183.
Publication history
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Publication history

Received: 24 December 2019
Revised: 22 May 2020
Accepted: 22 May 2020
Published: 28 July 2020
Issue date: August 2020

Copyright

© The Author(s) 2020

Acknowledgements

This study was supported by the National Natural Science Foundation of China (Grant Nos. 61771104 and U1809215).

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