Dielectric and tunable characteristics of Ba0.4Sr0.6TiO3-BaWO4 composite ceramics for microwave applications

Phase compositions, microstructure and microwave dielectric properties, of BaWO₄ (BW)-Ba_0.4Sr_0.6TiO₃ (BST) composite ceramics, prepared by the traditional solid-state route, were systematically characterized. Meanwhile, mechanism of dielectric tunability of those materials was discussed. Dielectric properties of the BW-BST composites at a DC bias field near the phase transition temperature could be interpreted by using Johnson's phenomenological equation. The sample with x = 0.60 exhibited a tunability of 29.5%, a dielectric permittivity of 192 and a Q value of 231 (at 2.700 GHz), which make it a promising candidate for applications in electrically tunable microwave devices.     

Effect of MgWO4 content on properties of Ba0.5Sr0.5TiO3 composite ceramics for tunable microwave applications

xMgWO₄-(1 − x) Ba_0.5Sr_0.5TiO₃ (x = 0.0, 5.0, 15.0, 25.0 and 35.0 wt%) composite ceramics were prepared via solid state reaction processing. Their structural and dielectric properties were systematically characterized. A significant increase in grain size was observed with increasing MgWO₄ content, which was accompanied by obvious variations in dielectric properties of the composite ceramics. It is found that the permittivity peaks of the samples gradually shifted to low temperatures with increasing MgWO₄ content. At the same time, tunabilities of the composite ceramics decreased, but their Q values increased. The sample with 35 wt% MgWO₄ possesses a high tunability of 16.8% (∼10 kHz), a low permittivity of 65 and an appropriate Q value of 309 (∼4.303 GHz), which meet the requirements of high power and impedance matching, thus making it a promising candidate for applications as electrically tunable microwave devices.     

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.     

High dielectric tunability of Ba0.6Sr0.4TiO3 thin film deposited by radio-frequency magnetron sputtering

In microwave tunable devices, one of the major challenges encountered is the simultaneous minimization of the material's dielectric loss and maximization of dielectric tunability. In this work, Ba_0.6Sr_0.4TiO₃ thin film with the thickness of 300 nm was deposited on Pt/SiO₂/Si substrates using radio-frequency magnetron sputtering technique, and its dielectric properties were investigated. Due to the high temperature annealing process at substrate temperature of 600 °C, well-crystallized Ba_0.6Sr_0.4TiO₃ film was deposited. The dielectric constant and dielectric loss of the film at 100 kHz are 300 and 0.033, respectively. Due to the good crystallinity of the Ba_0.6Sr_0.4TiO₃ films deposited by radio-frequency magnetron sputtering, high dielectric tunability up to 38.3% is achieved at a low voltage of 4.5 V.     

Dielectric and piezoelectric properties of Y2O3 doped (Bi0.5Na0.5)0.94Ba0.06TiO3 lead-free piezoelectric ceramics

Y₂O₃ doped lead-free piezoelectric ceramics (Bi_0.5Na_0.5)_0.94Ba_0.06TiO₃ (0-0.7 wt%) were synthesized by the conventional solid state reaction method, and the effect of Y₂O₃ addition on the structure and electrical properties was investigated. X-ray diffraction shows that Y₂O₃ diffuses into the lattice of (Bi_0.5Na_0.5)_0.94Ba_0.06TiO₃ to form a solid solution with a pure perovskite structure. The temperature dependence of dielectric constant of Y₂O₃ doped samples under various frequencies indicates obvious relaxor characteristics different from typical relaxor ferroelectric and the mechanism of the relaxor behavior was discussed. The optimum piezoelectric properties of piezoelectric constant d₃₃ = 137 pC/N and the electromechanical coupling factor k_p = 0.30 are obtained at 0.5% and 0.1% Y₂O₃ addition, respectively.     

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.     

Improved microwave dielectric properties of B2O3-doped Nd(Co1/2Ti1/2)O3 ceramics with near zero temperature coefficient of resonant frequency

The microwave dielectric properties and the microstructures of Nd(Co_1/2Ti_1/2)O₃ ceramics prepared by conventional solid-state route have been studied. The prepared Nd(Co_1/2Ti_1/2)O₃ exhibited a mixture of Co and Ti showing 1:1 order in the B-site. It is found that low-level doping of B₂O₃ (up to 0.75 wt.%) can significantly improve the density and dielectric properties of Nd(Co_1/2Ti_1/2)O₃ ceramics. Nd(Co_1/2Ti_1/2)O₃ ceramics with additives could be sintered to a theoretical density higher than 98.5% at 1320 °C. Second phases were not observed at the level of 0.25-0.75 wt.% B₂O₃ addition. The temperature coefficient of resonant frequency (τ_f) was not significantly affected, while the dielectric constants (?_r) and the unloaded quality factors Q were effectively promoted by B₂O₃ addition. At 1320 °C/4 h, Nd(Co_1/2Ti_1/2)O₃ ceramics with 0.75 wt.% B₂O₃ addition possesses a dielectric constant (?_r) of 27.2, a Q × f value of 153,000 GHz (at 9 GHz) and a temperature coefficient of resonant frequency (τ_f) of 0 ppm/°C. The B₂O₃-doped Nd(Co_1/2Ti_1/2)O₃ ceramics can find applications in microwave devices requiring low sintering temperature.     

Dielectric properties of (1−x)(Mg0.95Co0.05)TiO3-xCaTiO3 ceramic system at microwave frequency

The microwave dielectric properties and the microstructures of the (1−x)MgTiO₃-xCaTiO₃ ceramic system were investigated. With partial replacement of Mg by Co, dielectric properties of the (1−x)(Mg_0.95Co_0.05)TiO₃-xCaTiO₃ ceramics can be promoted. The microwave dielectric properties are strongly correlated with the sintering temperature. At 1275°C, the 0.95(Mg_0.95Co_0.05)TiO₃-0.05CaTiO₃ ceramics possesses excellent microwave dielectric properties: a dielectric constant ε_r of 20.3, a Q×f value of 107 000 ( at 7 GHz) and a τ_f value of −22.8 ppm/°C. By appropriately adjusting the x value in the (1−x)(Mg_0.95Co_0.05)TiO₃-xCaTiO₃ ceramic system, zero τ_f value can be achieved. With x=0.07, a dielectric constant ε_γ of 21.6, a Q×f value of 92 000 (at 7 GHz) and a τ_f value of −1.8 ppm/°C was obtained for 0.93(Mg_0.95Co_0.05)TiO₃-0.07CaTiO₃ ceramics sintered at 1275°C for 4 h.     

Modified tunable dielectric properties by addition of MgO on BaZr0.25Ti0.75O3 ceramics

Phase composition, microstructure and tunable dielectric properties of (1 − x)BaZr_0.25Ti_0.75O₃-xMgO (BZTM) composite ceramics fabricated by solid-state reaction were investigated. It was found Mg not only existed in the matrix as MgO, there was also trace amount of Mg²⁺ ions dissolved in the BZT grains, which led to Curie temperature of the BZTM composites ceramics shifting to below −100 °C. Dielectric permittivity of the BZTM composite ceramics was reduced from thousands to hundreds by manipulating the content of MgO. Johnson's phenomenological equation based on Devonshire's theory was used to describe the nonlinear dielectric permittivity of the ceramics with increasing applied DC field. With increasing content of MgO, anharmonic constant α_(T) increased monotonously. Dielectric permittivity was 672, while dielectric tunability was as high as 30.0% at 30 kV/cm and dielectric loss was around 0.0016 for the 0.6BaZr_0.25Ti_0.75O₃-0.4MgO sample at 10 kHz and room temperature.     

Microstructures and dielectric properties of Ba0.5Sr0.5TiO3–Zn2TiO4 composite ceramics with low sintering temperature for tunable device applications

Ba_0.5Sr_0.5TiO₃–Zn₂TiO₄ composite ceramics with low dielectric constant and high tunability are fabricated at a relatively low sintering temperature of 1200 °C via the conventional solid-state reaction route. Zn₂TiO₄ and Ba_0.5Sr_0.5TiO₃ can be friendly coexistent in the composite material system. The dielectric constant is tailored from 2500 to 83 by manipulating the addition of Zn₂TiO₄ content from 0 wt.% to 80 wt.% weight ratio. The dielectric loss still keeps around 0.002 and the tunability is 10.3% under a DC-applied electric field of 30 kV/cm at 10 kHz for the 80 wt.% Zn₂TiO₄ added Ba_0.5Sr_0.5TiO₃ composite ceramics. These composite ceramics are promising candidates for multilayer low-temperature co-fired ceramics (LTCC) and potential tunable devices applications.     

Microstructures and dielectric properties of Ba0.6Sr0.4TiO3-MgO ceramics prepared by non-aqueous gelcasting and dry pressing

Non-aqueous gelcasting and dry pressing were used to prepare 45 wt% Ba_0.6Sr_0.4TiO₃-55 wt% MgO (BSTM) ceramics. The effects of different forming methods on the microstructures and dielectric properties of the BSTM ceramics were investigated. The densities of the BSTM ceramics prepared by non-aqueous gelcasting are lower but more uniform than that of the BSTM ceramics prepared by dry pressing. The XRD analysis illustrates that phase compositions are completely the same no matter what forming method is adopted. The SEM results show that the BSTM green samples and sintered ceramics prepared by non-aqueous gelcasting are more uniform than that prepared by dry pressing. Furthermore, it is found that the BSTM ceramics prepared by non-aqueous gelcasting have higher and more uniform dielectric constant, tunability and loss tangent (measured at 10 kHz and 20 °C). Meanwhile, the BSTM ceramics prepared by non-aqueous gelcasting have higher dielectric constant and lower Q × f value (namely more loss) when they are measured at microwave frequencies.     

Processing, dielectric properties and impedance characteristics of Na0.5Bi0.5Cu3Ti4O12 ceramics

Na_0.5Bi_0.5Cu₃Ti₄O₁₂ (NBCTO) ceramics were prepared by conventional solid-state reaction method. The phase structure, microstructure and dielectric properties of NBCTO ceramics sintered at various temperatures with different soaking time were investigated. Pure NBCTO phase could be obtained with increasing the temperature and prolonging the soaking time. High dielectric permittivity (13,495) and low dielectric loss (0.031) could be obtained when the ceramics were sintered at 1000 °C for 7.5 h. The ceramics sintered at 1000 °C for 7.5 h also showed good temperature stability (−4.00 to −0.69%) over a large temperature range from −50 to 150 °C. Complex impedances results revealed that the grain was semiconducting and the grain boundaries was insulating. The grain resistance (R_g) was 12.10 Ω cm and the grain boundary resistance (R_gb) was 2.009 × 10⁵ Ω cm when the ceramics were sintered at 1000 °C for 7.5 h.     

Structure and electrical properties of (1 − x)Bi0.5Na0.5TiO3-xBi0.5K0.5TiO3 ceramics near morphotropic phase boundary

The binary lead-free piezoelectric ceramics with the composition of (1 − x)Bi_0.5Na_0.5TiO₃-xBi_0.5K_0.5TiO₃ were synthesized by conventional mixed-oxide method. The phase structure transformed from rhombohedral to tetragonal phase in the range of 0.16 ≤ x ≤ 0.20. The grain sizes varied with increasing the Bi_0.5K_0.5TiO₃ content. Electrical properties of ceramics are significantly influenced by the Bi_0.5K_0.5TiO₃ content. Two phase transitions at T_t (the temperature at which the phase transition from rhombohedral to tetragonal occurs) and T_c (the Curie temperature) were observed in all the ceramics. Adding Bi_0.5K_0.5TiO₃ content caused the variations of T_t and T_c. A diffuse character was proved by the linear fitting of the modified Curie-Weiss law. Besides, the ceramics with homogeneous microstructure and excellent electrical properties were obtained at x = 0.18 and sintered at 1170 °C. The piezoelectric constant d₃₃, the electromechanical coupling factor K_p and the dielectric constant ?_r reached 144 pC/N, 0.29 and 893, respectively. The dissipation factor tan δ was 0.037.     

Enhancement microwave dielectric properties of La(Mg0.5Sn0.5)O3 ceramics by Substituting Mg for Co

The microwave dielectric properties of La(Mg_0.5−xCo_xSn_0.5)O₃ ceramics were examined with a view to exploiting them for mobile communication. The La(Mg_0.5−xCo_xSn_0.5)O₃ ceramics were prepared using the conventional solid-state method with various sintering temperatures. The X-ray diffraction patterns of the La(Mg_0.4Co_0.1Sn_0.5)O₃ ceramics revealed that La(Mg_0.4Co_0.1Sn_0.5)O₃ is the main crystalline phase, which is accompanied by small extent of La₂Sn₂O₇ as the second phase. Formation of this Sn-rich second phase was attributed to the loss of MgO upon ignition. Increasing the sintering temperatures seemed to promote the formation of La₂Sn₂O₇. An apparent density of 6.67 g cm⁻³, a dielectric constant (?_r) of 20.3, a quality factor (Q.F.) of 70,500 GHz, and a temperature coefficient of resonant frequency (τ_f) of −77 ppm °C⁻¹ were obtained for La(Mg_0.4Co_0.1Sn_0.5)O₃ ceramics that were sintered at 1550 °C for 4 h.     

Preparation, characterization and microwave absorption properties of polyaniline/Co0.5Zn0.5Fe2O4 nanocomposite

The polyaniline (PAni)/Co_0.5Zn_0.5Fe₂O₄ nanocomposite was prepared by an in situ polymerization in an aqueous solution. The products were characterized by Fourier transform infrared (FT-IR) spectrometer, ultraviolet-visible (UV-vis) spectrometer, X-ray diffraction (XRD) and transmission electron microscope (TEM). The average particle size of the PAni/Co_0.5Zn_0.5Fe₂O₄ was estimated to be about 70 nm by TEM. The reflection loss (dB) of the nanocomposite was measured at different microwave frequencies in X-band (8.2-12.4 GHz), U-band (12.4-18 GHz) and K-band (18-26.5 GHz) by radar cross-section (RCS) method according to the national standard GJB-2038-94. The results showed the reflection loss of the PAni/Co_0.5Zn_0.5Fe₂O₄ nanocomposite was higher than that of the PAni. The maximum reflection loss of the PAni/Co_0.5Zn_0.5Fe₂O₄ nanocomposite was about −39.9 dB at 22.4 GHz with a bandwidth of 5 GHz (full frequency width at about a half of the peak response). In conclusion, this sample is a good microwave shielding and absorbing materials at higher frequency.     

Effect of B-site doping on Sm0.5Sr0.5MxCo1−xO3−δ properties for IT-SOFC cathode material (M = Fe, Mn)

The crystal structure, thermal expansion rate, electrical conductivity and electrochemical performance of Sm_0.5Sr_0.5M_xCo_1−xO_3−δ (M = Fe, Mn) have been investigated. Two crystal structures have been observed in the specimens of Sm_0.5Sr_0.5Fe_xCo_1−xO_3−δ (SSFC) at room temperature, the perovskite structure of SSFC has an orthorhombic symmetry for 0 ≤ x ≤ 0.4 and a cubic symmetry for 0.5 ≤ x ≤ 0.9. The specimens of Sm_0.5Sr_0.5Mn_xCo_1−xO_3−δ (SSMC) crystallize in an orthorhombic structure. The adjustment of thermal expansion rate to electrolyte, which is one of the main problems of SSC, can be achieved to lower TEC values with more Fe and Mn substitution. Especially, Sm_0.5Sr_0.5Mn_0.8Co_0.2O_3−δ exhibits good thermal compatibility with La_0.8Sr_0.2Ga_0.8Mg_0.2O₃. High electrical conductivities are obtained for all the specimens and they demonstrate above 100 S/cm at 800 °C in SSFC system. The polarization resistance increases with increasing Mn content, Nevertheless, the polarization resistance of SSFC increases with increasing Fe content, but when the amount of Fe reaches to 0.4, the maximum is obtained while the resistance will decrease when the amount of Fe reaches above 0.4. Sm_0.5Sr_0.5Fe_0.8Co_0.2O_3−δ electrode exhibits high catalytic activity for oxygen reduction operating at temperature from 700 to 800 °C.     

Structure and ferroelectric properties in (K0.5Bi0.5)TiO3-BiScO3-PbTiO3 piezoelectric ceramic system

(K_0.5Bi_0.5)TiO₃-BiScO₃-PbTiO₃ ceramics were synthesized by conventional solid-state method. A morphotropic phase boundary (MPB) was confirmed with the aid of structural analysis. Two dielectric anomalous peaks were observed, the one around dielectric maximum temperature (T_m) due to phase transformation from ferroelectric to paraelectric while the second one could be ascribed to space charges. Furthermore, the existence of space charges also resulted in the independence of T_m with frequency at low lead composition. A new high temperature piezoelectric ceramic, 0.30(K_0.5Bi_0.5)TiO₃-0.30BiScO₃-0.40PbTiO₃ close to MPB exhibited excellent electrical properties with T_m of 384 °C, d₃₃ of 247 pC/N, k_p of 38.9%, P_r of 19.41 μC/cm², and E_c of 2.25 kV/mm, indicative of a candidate for high temperature application.     

Synthesis and characterization of (Na0.85K0.15)0.5Bi0.5TiO3 ceramics by different methods

The (Na_0.85K_0.15)_0.5Bi_0.5TiO₃ (BNKT) powders were synthesized by solid-state method, sol-gel method and stearic acid method. Microstructure, piezoelectric and dielectric properties of the ceramics were investigated. Attempts had been made to understand the reaction processes by using thermo gravimetric (TG) and differential scanning calorimetry (DSC). The BNKT powders have a perovskite structure with average crystallite sizes of 168 nm, 85 nm and 79 nm, corresponding to the solid-state method, the sol-gel method and the stearic acid method, respectively. The ceramics derived from the powder synthesized by sol-gel method presents the most homogeneous microstructure and largest grain size (5-7 μm). The effects of average crystallite size on microstructures and electric properties of the BNKT ceramics were investigated. Both the piezoelectric properties and dielectric properties were enhanced with the increase of grain size.     

Dielectric properties and substitution mechanism of samarium-doped Ba0.68Sr0.32TiO3 ceramics

Ba_0.68Sr_0.32TiO₃ ceramics of perovskite structure are prepared by solid state reaction method with addition of x mol% Sm₂O₃, and their dielectric properties are investigated. It is found that, integrating with the lattice parameters and tolerance factor t, there is an alternation of substitution preference of Sm³⁺ for the host cations in perovskite lattice. Owing to the replacement of Sm³⁺ ions for Ba²⁺ ions in the A site, T_c rises with the increase of Sm₂O₃ doping when the doping content is below 0.1 mol%; meanwhile, when the content is more than 0.1 mol%, Sm³⁺ ions tend to occupy the B-site, causing a drop of T_c. Owing to the modifications of Sm³⁺ doping, dielectric constant, dissipation factor and temperature stability of dissipation factor are influenced remarkably, making it a superior candidate for environment-friendly applications. Moreover, the creation of oxygen vacancies controls the dielectric constant when the addition is above 0.1 mol%, so the dielectric constant decreases with increasing of samarium.     

Optimized microwave dielectric properties of Co- and Ca-substituted Mg0.6Zn0.4TiO3

The system of (1 − y)(Mg_0.6Zn_0.4)_1−xCo_xTiO₃-yCaTiO₃ was investigated to optimize its microwave dielectric properties by adopting appropriate contents of Co and Ca and by controlling sintering conditions. The effect of Co substitution was to enhance densification and Qf value, while the addition of CaTiO₃ resulted in increases of dielectric constant and TCF. As an optimal compositions, 0.93(Mg_0.6Zn_0.4)_0.95Co_0.05TiO₃-0.07CaTiO₃ successfully demonstrated a dielectric constant of 23.04, a Qf of 79,460 GHz and a TCF value of +1.4 ppm/°C after firing at a relatively lower sintering temperature of 1200 °C. The increase of sintering temperature beyond 1200 °C tended to degrade overall microwave dielectric properties presumably due to Zn volatilization as evidenced by the presence of a Zn-deficient phase (MgTi₂O₅) at 1400 °C. An attempt to establish the correlation between microstructure characteristics and dielectric properties was made in this dielectric system where the extensive range of firing temperature up to 1400 °C was evaluated.