Low-temperature sintering and compatibility with silver electrode of Ba4MgTi11O27 microwave dielectric ceramic

Ba₄MgTi₁₁O₂₇ microwave dielectric ceramic was investigated using X-ray diffraction, scanning electron microscopy and dielectric measurement. The pure Ba₄MgTi₁₁O₂₇ ceramic shows a high sintering temperature (∼1275 °C) and good microwave dielectric properties as Q × f of 19,630 GHz, ?_r of 36.1, τ_f of 14.6 ppm/°C. It was found that the addition of BaCu(B₂O₅) (BCB) can effectively lower the sintering temperature from 1275 to 925 °C, and does not induce much degradation of the microwave dielectric properties. The BCB-doped Ba₄MgTi₁₁O₂₇ ceramics can be compatible with Ag electrode, which makes it a promising ceramic for LTCC technology application.     

A low-firing microwave dielectric material in Li2O-ZnO-Nb2O5 system

LiZnNbO₄ ceramic was fabricated by the conventional solid state reaction method and its microwave dielectric properties were reported for the first time. The phase structure, microstructure, and sintering behavior were also investigated. The LiZnNbO₄ ceramic could be well densified at around 950 °C and demonstrated high performance microwave dielectric properties with a low relative permittivity ~ 14.6, a high quality factor (resonant frequency/dielectric loss) ~ 47, 200 GHz (at 8.7 GHz), and a negative temperature coefficient of resonant frequency approzmiately −64.5 ppm/°C. The LiZnNbO₄ ceramic is chemically compatible with Ag electrode material at its sintering temperature. It can be a promising microwave dielectric material for low-temperature co-fired ceramic technology.     

Low temperature sintering and microwave dielectric properties of ZnTiNb2O8 ceramics with BaCu(B2O5) additions

The phases, microstructure and microwave dielectric properties of ZnTiNb₂O₈ ceramics with BaCu(B₂O₅) additions prepared by solid-state reaction method have been investigated using X-ray diffraction (XRD) and scanning electron microscopy (SEM). The pure ZnTiNb₂O₈ ceramic shows a high sintering temperature of about 1250 °C. However, it was found that the addition of BaCu(B₂O₅) lowered the sintering temperature of ZnTiNb₂O₈ ceramics from above 1250 °C to 950 °C due to the BCB liquid-phase. The results showed that the microwave dielectric properties were strongly dependent on densification, crystalline phases and grain size. Addition of 3 wt% BCB in ZnTiNb₂O₈ ceramics sintered at 950 °C afforded excellent dielectric properties of ?_r = 32.56, Q × f = 20,100 GHz (f = 5.128 GHz) and τ_f = −64.87 ppm/°C. These represent very promising candidates for LTCC dielectric materials.     

Low-temperature firing and microwave dielectric properties of ZnO-Nb2O5-TiO2-SnO2 ceramics with CuO-V2O5

The effects of CuO-V₂O₅ addition on the sintering temperature and microwave dielectric properties of ZnO-Nb₂O₅-TiO₂-SnO₂ were investigated. The CuO-V₂O₅ addition lowered the sintering temperature of ZnO-Nb₂O₅-TiO₂-SnO₂ ceramics effectively from 1150 to 860 °C due to the liquid-phase effect of Cu₂V₂O₇ and Cu₃(VO₄)₂, as observed by XRD. The microwave dielectric properties were found to strongly correlate with the sintering temperature and the amount of CuO-V₂O₅ addition. The maximum Qf values decreased with increasing CuO-V₂O₅ content, due to the formation of the second phase, Cu₃(VO₄)₂ and CuNbO₃. Zero τ_f value can be obtained by properly adjusting the sintering temperature. At 860 °C, ZnO-Nb₂O₅-TiO₂-SnO₂ ceramics with 1.5 wt.% CuO-V₂O₅ gave excellent microwave dielectric properties: ?_r = 42.3, Qf = 9000 GHz and τ_f = 8 ppm/°C.     

Microwave dielectric properties and microstructures of the 11Li2O-3Nb2O5-12TiO2 ceramics with B2O3 addition

The effects of B₂O₃ addition, as a sintering agent, on the sintering behavior, microstructure and microwave dielectric properties of the 11Li₂O-3Nb₂O₅-12TiO₂ (LNT) ceramics have been investigated. With the low-level doping of B₂O₃ (≤2 wt.%), the sintering temperature of the LNT ceramic could be effectively reduced to 900 °C. The B₂O₃-doped LNT ceramics are also composed of Li₂TiO₃ss and “M-phase” phases. No other phase could be observed in the 0.5-2 wt.% B₂O₃-doped ceramics sintered at 840-920 °C. The addition of B₂O₃ induced no obvious degradation in the microwave dielectric properties but increased the τ_f values. Typically, the 0.5 wt.% B₂O₃-doped ceramics sintered at 900 °C have better microwave dielectric properties of ?_r = 49.2, Q × f = 8839 GHz, τ_f = 57.6 ppm/°C, which suggest that the ceramics could be applied in multilayer microwave devices requiring low sintering temperatures.     

Effect of B2O3-Bi2O3-SiO2-ZnO glass on the sintering and microwave dielectric properties of 0.83ZnAl2O4-0.17TiO2

The 0.83ZnAl₂O₄-0.17TiO₂ (ZAT) ceramics were synthesized by solid state ceramic route. The effect of 27B₂O₃-35Bi₂O₃-6SiO₂-32ZnO (BBSZ) glass on the microwave dielectric properties of ZAT was investigated. The crystal structure and the microstructure of the ceramic-glass composites were studied by X-ray diffraction and scanning electron microscopic techniques. The low frequency dielectric loss was measured at 1 MHz. The dielectric properties of the sintered samples were measured in the microwave frequency range by the resonance method. Addition of 0.2 wt% of BBSZ improved the dielectric properties with quality factor (Q_u × f) > 120,000 GHz, temperature coefficient of resonant frequency (τ_f) = −7.3 ppm/°C and dielectric constant (?_r) = 11.7. Addition of 10 wt% of BBSZ lowered the sintering temperature to about 950 °C with Q_u × f > 10,000 GHz, ?_r = 10 and τ_f = −23 ppm/°C. The reactivity of 10 wt% BBSZ added ZAT with silver was also studied. The results show that ZAT doped with suitable amount of BBSZ glass is a possible material for low-temperature co-fired ceramic (LTCC) application.     

Study on properties of CaO-SiO2-B2O3 system glass-ceramic

Low temperature co-fired ceramic (LTCC) is prepared by sintering a glass selected from CaO-SiO₂-B₂O₃ system, and its sintered bodies are characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy dispersive spectroscopy (EDS). It is found that the optimal sintering temperature for this glass-ceramic is 820 °C for 15 min, and the major phases of this material are CaSiO₃, CaB₂O₄ and SiO₂. The glass-ceramic possesses excellent dielectric properties: ?_r = 6.5, tan δ < 2 × 10⁻³ at 10 MHz, temperature coefficient of dielectric constant about −51 × 10⁻⁶ °C⁻¹ and coefficient of thermal expansion about 8 × 10⁻⁶ °C⁻¹ at 20-400 °C. Thus, this material is supposed to be suitable for the tape casting process and be compatible with Ag electrode, which could be used as the LTCC materials for the application in wireless communications.     

Temperature compensated Sr2Al2SiO7 ceramic for microwave applications

The Sr–Gehlenite (Sr₂Al₂SiO₇) ceramic has been prepared by the conventional solid-state ceramic route. Phase pure Sr₂Al₂SiO₇ (SAS) ceramic sintered at 1525 °C for 4 h has ?_r = 7.2 and Q_u × f = 33,000 GHz. The SAS showed large negative τ_f of −37.0 ppm/ °C. A low value of τ_f was achieved by preparing SAS–CaTiO₃ composite. The composite with 0.04 volume fractions (V_f) CaTiO₃ sintered at 1500 °C for 4 h showed good microwave dielectric properties: ?_r = 8.6, Q_u × f = 20,400 GHz and τ_f = +8.5 ppm/°C.     

Microwave dielectric properties of LaMgAl11O19

The suitable choice of a substrate material is one of the aims to be fulfilled in high speed microwave technology. LaMgAl₁₁O₁₉ oxide ceramic material, which belongs to the magnetoplumbite family, has been reported earlier as a potential candidate for such applications. This material has been prepared by conventional solid-state ceramic route. The structure has been studied by X-ray diffraction and characterized at microwave frequencies. The effect of dopant and glass addition on the microwave dielectric properties of this material has also been investigated. LaMgAl₁₁O₁₉ has relatively low dielectric constant (ε_r=14), low dielectric loss or high quality factor (Q_u×f>28,000 GHz at 7 GHz) and small temperature variation of resonant frequency (τ_f=−12 ppm/°C) at room temperature (300 K). These properties make LaMgAl₁₁O₁₉ as a good substrate material and as a dielectric resonator to be used in microwave devices operating at relatively high frequencies.     

Microwave dielectric in the Sm(Co1/2Ti1/2)O3-CaTiO3 ceramic system with near-zero temperature coefficient with resonant frequency

The ceramic system prepared by the conventional solid state method was investigated for its microstructures and microwave dielectric properties. To achieve a temperature-stable material, two compounds with negative and positive temperature coefficients were employed to form mixed phases. The microwave dielectric properties are strongly correlated with composition. For practical application, a dielectric constant (ε_r) of 37, a quality factor (Q × f value) of 43,000 GHz and a temperature coefficient of resonant frequency (τ_f) of 1 ppm/°C for 0.6Sm(Co_1/2Ti_1/2)O₃-0.4CaTiO₃ sintered at 1420 °C are proposed.     

Study of the dielectric properties in the NaNbO3 -KNbO3-In2O3 system using AC impedance spectroscopy

We report a comparative study of the dielectric properties of solid-state (ceramic method) synthesized NaNbO₃ (NN), Na_0.75K_0.25NbO₃ (K25NN), K_0.5Na_0.5NbO₃ (KNN) and some composite materials containing In₂O₃ and NN or KNN using an AC impedance method. Powder X-ray diffraction (PXRD) was employed to investigate the phase purity. No significant amount of impurity phase was observed for NN, K25NN, and KNN. Substitutions of 10, 15 and 25 mol% In³⁺ for Nb⁵⁺ in KNN and NN using solid-state reactions at 1150 °C resulted in composite materials. AC impedance studies of NN, KNN and K25NN in the temperature range of 500-800 °C showed a single semicircle (attributed to the bulk property) in the high-frequency range of 10³ to 10⁶ Hz. The individual contributions from the bulk and grain boundary on the dielectric properties were resolved and quantified from the impedance data. The calculated dielectric values for NN were consistent with previously reported in the literature. 10% Indium based KNN composite materials had the lowest dielectric loss 0.585 and the dielectric constant of 233 at 100 kHz at the temperature of 650 °C.     

Ba2Ti9O20-Ba1.85Sm4.1Ti9O24 layered dielectric resonators with adjustable effective dielectric constant

The layered dielectric resonator structures composed of Ba₂Ti₉O₂₀ (BTO) and Ba_1.85Sm_4.1Ti₉O₂₄ (BSTO) ceramic pellets were introduced to design new microwave dielectric materials with adjustable dielectric constant between 50 and 70. Good combination of microwave dielectric properties (?_r,eff = 50 ~ 70, Qf = 11,700-19,100 GHz and τ_f = − 4.3 to − 1.5 ppm/°C) was obtained by the present approach, and such combination could be optimized by adjusting the volume fraction of BSTO and stacking scheme. For practical applications, the BTO and BSTO layers could be bonded by low-loss adhesive, and the effects of the adhesive on the microwave dielectric properties were limited.     

Dielectric properties of a new ceramic system (1 − x)Mg4Nb2O9-xCaTiO3 at microwave frequency

The microstructures and the microwave dielectric properties of the (1 − x)Mg₄Nb₂O₉-xCaTiO₃ ceramic system were investigated. In order to achieve a temperature-stable material, CaTiO₃ (τ_f ∼ 800 ppm/°C) was chosen as a τ_f compensator and added to Mg₄Nb₂O₉ (τ_f ∼ −70 ppm/°C) to form a two phase system. It was confirmed by the XRD and EDX analysis. By appropriately adjusting the x-value in the (1 − x)Mg₄Nb₂O₉-xCaTiO₃ ceramic system, near-zero τ_f value can be achieved. A new microwave dielectric material, 0.5Mg₄Nb₂O₉-0.5CaTiO₃ applicable in microwave devices is suggested and possesses the dielectric properties of a dielectric constant ?_r ∼ 24.8, a Q × f value ∼82,000 GHz (measured at 9.1 GHz) and a τ_f value ∼−0.3 ppm/°C.     

Improved high-Q microwave dielectric resonator using CuO-doped MgNb2O6 ceramics

The microwave dielectric properties and the microstructures of MgNb₂O₆ ceramics with CuO additions (1-4 wt.%) prepared with conventional solid-state route have been investigated. The sintered samples exhibit excellent microwave dielectric properties, which depend upon the liquid phase and the sintering temperature. It is found that MgNb₂O₆ ceramics can be sintered at 1140 °C due to the liquid phase effect of CuO addition. At 1170 °C, MgNb₂O₆ ceramics with 2 wt.% CuO addition possesses a dielectric constant (ε_r) of 19.9, a Q×f value of 110,000 (at 10 GHz) and a temperature coefficient of resonant frequency (τ_f) of −44 ppm/°C. The CuO-doped MgNb₂O₆ ceramics can find applications in microwave devices requiring low sintering temperature.     

Microwave dielectric properties of (ABi)1/2MoO4 (A = Li,Na, K,Rb, Ag) type ceramics with ultra-low firing temperatures

A series of (ABi)_1/2MoO₄ (A = Li, Na, K, Rb, Ag) compositions were studied in regard to the sintering behavior, phase composition, microwave dielectric properties and chemical compatibility with silver and/or aluminum for electrodes. All the (ABi)_1/2MoO₄ (A = Li, Na, K, Rb, Ag) ceramics could be sintered below 700 °C with relative densities above 93%. Whereas the (KBi)_1/2MoO₄ ceramic can be sintered to a high density at around 630 °C/2 hrs with a relative permittivity ∼37, a Qf value of 4000 GHz and a temperature coefficient of resonant frequency (TCF) ∼ +117 ppm/°C. Furthermore, from the XRD analysis of co-fired ceramics, the (KBi)_1/2MoO₄ ceramic reacts with silver but not with aluminum at its densification temperature. The (ABi)_1/2MoO₄ (A = Li, Na, K, Rb, Ag) type ceramics can all be considered into the new field of ultra-low temperature co-firing dielectrics for multilayer applications.     

Study on properties of BaxSmyTi7O20 ceramics with CaO-SiO2-B2O3 glass

The effect of CaO-SiO₂-B₂O₃ (CSB) glass addition on the sintering temperature and dielectric properties of Ba_xSm_yTi₇O₂₀ ceramics has been investigated using X-ray diffraction, scanning electron microscopy and differential thermal analysis. The CSB glass starts to melt at about 970 °C, and a small amount of CSB glass addition to Ba_xSm_yTi₇O₂₀ ceramics can greatly decrease the sintering temperature from about 1350 to about 1260 °C, which is attributed to the formation of liquid phase. It is found that the dielectric properties of Ba_xSm_yTi₇O₂₀ ceramics are dependent on the amount of CSB glass and the microstructures of sintered samples. The product with 5 wt% CSB glass sintered at 1260 °C is optimal in these samples based on the microstructure and the properties of sintering product, when the major phases of this material are BaSm₂Ti₄O₁₂ and BaTi₄O₉. The material possesses excellent dielectric properties: ?_r = 61, tan δ = 1.5 × 10⁻⁴ at 10 GHz, temperature coefficient of dielectric constant is −75 × 10⁻⁶ °C⁻¹.     

Synthesis and properties of Ba(Zn1/3Ta2/3)O3 for microwave and millimeter wave applications

High dielectric materials have gained an important position in microwave electronics by reducing the size and cost of components for a wide range of applications from mobile telephony to spatial communications. Ba(Zn_1/3Ta_2/3)O₃ (BZT) is an A(B′B″)O₃ type perovskite material, showing ultra high values of the quality factor Q. Ceramic-based BZT dielectric materials were prepared by solid state reaction. The samples were sintered at temperatures in the range 1400 ÷ 1600 °C for 4 h. Compositional, structural and morphological characterization were performed by using XRD, SEM and EDX analysis. The dielectric properties were measured in the microwave range (6 ÷ 7 GHz). An additional annealing at 1400 °C for 10 h has improved some dielectric parameters. For samples sintered at temperatures higher than 1500 °C, the permittivity values were obtained in the interval 30 ÷ 35 and almost do not change the value after the annealing. The Q × f product substantially increases up to about 135,000 GHz, exhibiting a low temperature coefficient of the resonant frequency (τ_f) in microwaves. The best parameters were obtained for the samples sintered at 1600 °C with additional annealing. The achieved high values of the Q × f product recommend these materials for microwave and millimeter wave applications.     

Structural and electrical properties of Na2Pb2Eu2W2Ti4X4O30 (X = Nb, Ta) ferroelectric ceramics

A new group of tungsten bronze family Na₂Pb₂Eu₂W₂Ti₄X₄O₃₀ (X = Nb, Ta) having all the valence elements (I-VI) were prepared by a high-temperature solid-state reaction technique. The formations of the compounds were confirmed by X-ray diffraction technique with an orthorhombic structure. Surface morphology of the compounds was studied by scanning electron microscope (SEM). Studies of dielectric properties (?_r and tan δ) of the above compounds at different frequencies in a wide temperature range (300-700 K) with an impedance analyzer exhibit a ferroelectric phase transition at 580 and 394 K for Na₂Pb₂Eu₂W₂Ti₄Nb₄O₃₀ and Na₂Pb₂Eu₂W₂Ti₄Ta₄O₃₀, respectively. Ferroelectric properties of these compounds were confirmed with polarization (hysteresis) study.     

Influence of Bi2O3 and CuO addition on low-temperature sintering and dielectric properties of Ba0.6Sr0.4TiO3 ceramics

In this study, we tried to lower the sintering temperature of Ba_0.6Sr_0.4TiO₃ (BST) ceramics by several kinds of adding methods of Bi₂O₃, CuO and CuBi₂O₄ additives. The effects of different adding methods on the microstructures and the dielectric properties of BST ceramics have been studied. In the all additive systems, the single addition of CuBi₂O₄ was the most effective way for lowering the sintering temperature of BST. When CuBi₂O₄ of 0.6 mol% was mixed with starting BST powders and sintered at 1100 °C, the derived ceramics demonstrated dense microstructure with a low dielectric constant (? = 4240), low dielectric loss (tan δ = 0.0058), high tunability (Tun = 38.3%) and high Q value (Q = 251). It was noteworthy that the sintering temperature was significantly lowered by 350 °C compared with no-additive system, and the derived ceramics maintained the excellent microwave dielectric properties corresponding to pure BST.     

Effect of sintering time on crystal structure and microwave dielectric properties in aeschynite-structured (Sm1−xYx)(Ti1.5W0.5)O6 (x = 0 and 0.5) ceramics

The crystal structure and microwave dielectric properties of the (Sm_1−xY_x)(Ti_1.5W_0.5)O₆ (x = 0 and 0.5) ceramics sintered at 1375 °C for 2-50 h were investigated in this study. No secondary phase was observed in the samples sintered for various sintering times, whereas a secondary phase was formed in the (Sm_0.5Y_0.5)(Ti_1.5W_0.5)O₆ ceramic sintered at 1400 °C for 50 h. As for the microstructure analysis, the formation of the liquid phase was observed in the both of the samples sintered for 20 and 50 h. The formation of the liquid phase is related to the compositional change of Ti and W from the stoichiometric composition of the samples caused by the instability of crystal structure. The dielectric constants were increased with increased sintering time in the both of the samples, though variations in the temperature coefficient of resonant frequency of the samples were not recognized with the variation in the sintering time. Moreover, although the quality factors of the each sample increased with increasing the sintering time from 2 to 10 h, decreases in the quality factors were recognized when the sintering time was over 10 h.