Synthesis and microwave dielectric properties of Ba4Ti3P2O15 ceramics

Present work introduces a new kind of microwave dielectric ceramic, Ba₄Ti₃P₂O₁₅. Ba₄Ti₃P₂O₁₅ ceramic can be prepared by solid state reaction method and be well densified after being sintered at above 1175 °C for 4 h in air. All the XRD patterns can be fully indexed as single-phase structure. The best microwave dielectric properties can be obtained in ceramic sintered at 1200 °C for 4 h with permittivity about 20.7, Q × f about 42,210 GHz and TCF about 37 ppm °C^?1. Measurements of the microwave dielectric properties of Ba₄Ti₃P₂O₁₅ ceramic revealed the existence of a maximum in the temperature dependence of the dielectric loss because of the defect dipoles relaxation.     

Low temperature sintering and microwave dielectric properties of Ba4Sm9.33Ti18O54 ceramics

The effect of BaCu(B₂O₅) (BCB) on the sinterability, microstructure and microwave dielectric properties of Ba₄Sm_9.33Ti₁₈O₅₄ (BST) has been investigated. Dilatometric measurements reveal that the sintering temperature of BST can be reduced by the addition of BCB. Microstructural analysis shows abnormal grain growth with large amount of BCB. A ceramic composite with Q × f = 4000 GHz, ?_r = 52 and τ_f = ?29 ppm/°C which can be sintered at 950 °C is obtained when 10 wt% BCB is added to BST. EDS analysis shows that the composite is chemically compatible with silver.     

Effect of BaCu(B2O5) on the sintering temperature and microwave dielectric properties of BaO–Ln2O3–TiO2 (Ln = Sm,Nd) ceramics

BaCu(B₂O₅) (BCB) ceramic powder was used to decrease the sintering temperatures of BaSm₂Ti₄O₁₂ (BST) and BaNd₂Ti₅O₁₄ (BNT) ceramics. The sintering temperature of the BST and BNT ceramics was reduced from approximately 1350 °C to 850 °C by the addition of BCB. The bulk density of the specimens increased and reached the saturated value with increasing BCB content. The variation of the dielectric constant (ɛ_r) was similar to that of the bulk density and, thus, the relative density plays an important role in determining the ɛ_r value of the specimens. The Q-value initially increased with the addition of BCB but decreased considerably when a large amount of BCB was added because of the presence of the liquid phase. Good microwave dielectric properties of Qxf = 4500 GHz, ɛ_r = 60 and τ_f = −30 ppm/°C were obtained for the 16.0 mol% BCB-added BST ceramics sintered at 875 °C for 2 h.     

Synthesis of the giant dielectric constant oxide CaCu3Ti4O12 via ethylenediaminetetraacetic acid precursor

CaCu₃Ti₄O₁₂ powders were prepared via EDTA route and single-phase CaCu₃Ti₄O₁₂ was obtained at 800 °C for 2 h. DTA/TG and XRD were used to characterize the precursor and derived oxide powders. The dielectric properties of CaCu₃Ti₄O₁₂ ceramics were presented. Increasing sintering temperature leads to the increase in dielectric constant. CaCu₃Ti₄O₁₂ ceramics sintered at 1090 °C for 3 h exhibited giant dielectric constant of up to 2.1 × 10⁵ at room temperature and 100 Hz, which is significantly higher than those obtained from other chemical methods.     

Influence of CuO addition to BaSm2Ti4O12 microwave ceramics on sintering behavior and dielectric properties

Microwave dielectric ceramics of tungsten–bronze-type BaSm₂Ti₄O₁₂ were prepared by doping CuO (up to 2 wt.%) as the liquid-phase sintering aid. The effects of CuO additive on the densification, micro structure and dielectric properties were investigated. Due to the liquid-phase effect, the sintering temperature of BaSm₂Ti₄O₁₂ ceramics with 1 wt.% CuO addition can be effectively reduced to 1160 °C, about 200 °C lower than that of pure BaSm₂Ti₄O₁₂ ceramics, while good microwave dielectric properties of ɛ_r = 75.8, Q*f = 4914.6 GHz and τ_f = −7.65 ppm/°C were still achieved.     

Effect of V2O5 additive to 0.4SrTiO3–0.6La(Mg0.5Ti0.5)O3 ceramics on sintering behavior and microwave dielectric properties

The effect of V₂O₅ addition on the microwave dielectric properties and the microstructures of 0.4SrTiO₃–0.6La(Mg_0.5Ti_0.5)O₃ ceramics sintered for 5 h at different sintering temperature were investigated systematically. It was found that the sintering temperature was effectively lowered about 200 °C by increasing V₂O₅ addition content. The grain sizes, bulk density as well as microwave dielectric properties were greatly dependent on sintering temperature and V₂O₅ content. The 4ST–6LMT ceramics with 0.25% V₂O₅ sintered at 1400 °C for 5 h in air exhibited optimum microwave dielectric properties of ɛ_r = 50.7, Q × f = 15049.6 GHz, T_f = −1.7 ppm/°C.     

Microwave dielectric properties of Ba(Mg1/3Ta(2−2x)/3Wx/3Tix/3)O3 ceramics

The microwave dielectric properties of ceramics based on Ba(Mg_1/3Ta_(2−2x)/3W_x/3Ti_x/3)O₃ is investigated as a function of x. The densification as well as dielectric properties deteriorate with increase in the substitution levels of (Ti_1/3W_1/3)^3.33+ at (Ta_2/3)^3.33+ site in Ba(Mg_1/3Ta_2/3)O₃. The τ_f is approaching zero between x = 0.1 and 0.15 in Ba(Mg_1/3Ta_(2−2x)/3W_x/3Ti_x/3)O₃ where quality factor is reasonably good (Q_u × f = 80,000–90,000 GHz). The Ba(Mg_1/3Ta_(2−2x)/3W_x/3Ti_x/3)O₃ with x = 1.0 has ɛ_r = 15.4, τ_f = −25.1 ppm/°C, Q_u × f = 35,400 GHz.     

Low-temperature firing and microwave dielectric properties of MgTiO3 ceramics with Bi2O3–V2O5

The effects of Bi₂O₃–V₂O₅ additive on the microstructures, the phase formation and the microwave dielectric properties of MgTiO₃ Ceramics were investigated. The Bi₂O₃–V₂O₅ addition lowered the sintering temperature of MgTiO₃ ceramics effectively from 1400 to 875 °C due to the liquid-phase effect. The microwave dielectric properties were found to strongly correlate with the amount of Bi₂O₃–V₂O₅ addition. The saturated dielectric constant decreased and the maximum Qf values increased with the increasing V₂O₅ content, which is attributed to the variation of the second phase including Bi₂Ti₂O₇, Bi₄V_1.5Ti_0.5O_10.85 and BiVO₄. At 875 °C, MgTiO₃ ceramics with 5.0 mol% Bi₂O₃–7 mol% V₂O₅ gave excellent microwave dielectric properties: ε_r = 20.6,Qf = 10420 GHz (6.3 GHz).     

Microwave dielectric properties of xNd(Zn1/2Ti1/2)O3–(1 − x)CaTiO3 ceramics

The microwave dielectric properties of xNd(Zn_1/2Ti_1/2)O₃–(1 − x)CaTiO₃ have been investigated. The system has been prepared by a conventional solid state ceramic route. Nd(Zn_1/2Ti_1/2)O₃ (NZT) possesses a dielectric constant (ε_r) of 32, a high quality factor (Q × f) of 170,000 GHz and a temperature coefficient of resonant frequency (τ_f) of − 42 ppm/°C. In order to produce a temperature-stable material, the addition of CaTiO₃ leads to a near-zero temperature variation of resonant frequency. In general, the microwave quality factor (Q × f) decreased as x increased and the temperature coefficient of resonant frequency (τ_f) was approximately linearly proportional to permittivity. The dielectric constant decreases from 77 to 32 as x varies from 0.2 to 1.0. The dielectric constant (ε_r) of 45, Q × f value of 56,000 (at 6 GHz) and temperature coefficient of resonant frequency (τ_f) of 0 ppm/°C were obtained for 0.5Nd(Zn_1/2Ti_1/2)O₃–0.5CaTiO₃ ceramics sintered at 1300 °C for 4 h. As the content of x increases, the highest Q × f value of 136,200 GHz for x = 0.8 is achieved at the sintering temperature 1300 °C.     

Ba2La2TiNb2O12: A new microwave dielectric of A4B3O12-type cation-deficient perovskites

A new A₄B₃O₁₂-type cation-deficient perovskite Ba₂La₂TiNb₂O₁₂ was prepared by the conventional solid-state reaction route. The phase and structure of the ceramics were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM). The compound crystallizes in the trigonal system with unit cell parameter a = 5.6726(3) Å, c = 27.740(2) Å, V = 773.04(9) ų and Z = 3. The microwave dielectric properties of the ceramic were studied using a network analyzer, and it shows a high dielectric constant of 42.70, a high quality factor with Q × f of 31,130 GHz, and a small negative τ_f of − 4.2 ppm °C^− 1.     

Modified giant dielectric properties of samarium doped CaCu3Ti4O12 ceramics

Effects of Sm³⁺ substitution on the microstructure and dielectric properties of CaCu₃Ti₄O₁₂ ceramics were investigated. The grain size of CaCu₃Ti₄O₁₂ ceramics was greatly decreased by doping with Sm³⁺, resulting from the ability of Sm³⁺ to inhibit the grain growth rate. This result can cause a decrease in the dielectric constant (?′) and loss tangent (tan δ) of CaCu₃Ti₄O₁₂ ceramics. Interestingly, high dielectric permittivity (?′ ～ 10,863) and low loss tangent (tan δ ～ 0.043 at 20 °C and 1 kHz) were observed in the Ca_0.925Sm_0.05Cu₃Ti₄O₁₂ ceramic. Nonlinear electrical properties of CaCu₃Ti₄O₁₂ ceramics were modified by doping with Sm³⁺. The dielectric relaxation behavior of Sm-doped CaCu₃Ti₄O₁₂ ceramics can be well ascribed based on the internal barrier layer capacitor model of Schottky barriers at the grain boundaries.     

Preparation and dielectric properties of Sr(Ti0.95Zr0.05)O3 ceramics doped with CaOTiO2SiO2 (CTS)

Sr(Ti_0.95Zr_0.05)O₃ ceramic was sintered using x mol.% CTS (x = 0, 0.5, 1.5, 4, 7) as sintering additive for the first time. Although Sr(Ti_0.95Zr_0.05)O₃ ceramic could not be fully sintered even at 1420 °C, the densification temperature could be decreased to 1280 °C by using CTS, which begin melting when temperature reaches higher than 1150 °C. The microstructures of the samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM). Apparent density and the dielectric properties were established at room temperature. The measuring frequency was 1 MHz. The microstructure and dielectric properties greatly changed depending on the amount of CTS additive. The optimum concentration to obtain nicer dielectric properties was 0.5 mol.%.     

Microwave dielectric properties and compatibility with silver of low-fired Ba2Ti3Nb4O18 ceramics with BaCu(B2O5) addition

The effects of BaCu(B₂O₅) (BCB) additions on the sintering temperature and microwave dielectric properties of Ba₂Ti₃Nb₄O₁₈ ceramic have been investigated. The addition of BCB can lower the sintering temperature of Ba₂Ti₃Nb₄O₁₈ ceramic from 1,250 to 900 °C and induce no obvious degradation of the microwave dielectric properties. Typically, the 5 wt% BCB added Ba₂Ti₃Nb₄O₁₈ ceramic sintered at 900 °C for 2 h exhibited good microwave dielectric properties of Q × f = 17,600 GHz, ε _r = 38.2 and τ _f  = 7 ppm/°C. The dielectric ceramic demonstrated stability against the reaction with the Ag electrode, which suggests that the ceramics could be applied in multilayer microwave devices requiring low sintering temperatures.     

Synthesis and characteristics of nature-superlattice-structured Bi3TiNbO9–Bi4Ti3O12 ferroelectric thin films by MOD

Natural-superlattice-structured ferroelectric thin films, Bi₃TiNbO₉–Bi₄Ti₃O₁₂ (BTN–BIT), have been synthesized on Pt/Ti/SiO₂/Si by metal organic decomposition (MOD) using BTN–BIT (1 mol:1 mol) solution. BTN–BIT films show natural-superlattice peaks below 2θ = 20° in X-ray diffraction patterns, which indicate that the BTN–BIT films annealed at 700–800 °C in O₂ ambient are consisted of iteration of two unit cells of Bi₃TiNbO₉ and one unit cell of Bi₄Ti₃O₁₂. As the annealing temperature increases from 600 to 750 °C, uniform and crack-free films, better crystallinity and ferroelectric properties can be obtained, but the pyrochlore phase in BTN–BIT films annealed over 800 °C would impair the ferroelectric properties. With the increase of O₂ flow rate from 0.5 to 1.5 L/min, both remanent polarization P_r and coercive electric field E_C increase, which are mainly attributed to reduction of the vacanvies of Bi and oxide ions in the films. Natural-superlattice-structured BTN–BIT thin films having 2–1 superlattice annealed at 750 °C in O₂ ambient with a flow rate of 1.5 L/min exhibit superior ferroelectric properties of P_r = 23.5 μC/cm² and E_C = 135 kV/cm.     

Effect of B2O3 and CuO additives on the sintering temperature and microwave dielectric properties of Ba(Mg1/3Nb2/3)O3 ceramics

B₂O₃ added Ba(Mg_1/3Nb_2/3)O₃ (BBMN) ceramics cannot be sintered below 930 °C. However, when CuO was added to them, they were sintered even at 850 °C. The amount of the Ba₂B₂O₅ second phase, which was formed in the BBMN ceramics decreased with the addition of CuO. Therefore, the CuO additive is considered to react with the B₂O₃ inhibiting the reaction between B₂O₃ and BaO. A dense microstructure without pores developed with the addition of a small amount of CuO. The bulk density, dielectric constant (ɛ_r) and Q-value increased with the addition of CuO, but decreased when a large amount of CuO was added. Excellent microwave dielectric properties were obtained for the Ba(Mg_1/3Nb_2/3)O₃ + 2.0 mol% B₂O₃ + 10.0 mol% CuO ceramic sintered at 875 °C for 2 h, with values Q_xf = 21 500 GHz, ɛ_r = 31 and temperature coefficient of resonance frequency (τ_f) = 21.3 ppm/°C.     

Phase formation and microwave dielectric properties of Pb2+ and Sr2+ doped La4Ti9O24 ceramics

Phase formation and microwave dielectric properties of the Pb²⁺ and Sr²⁺ doped La₄Ti₉O₂₄ ceramics were investigated. Using electron diffraction and Rietveld analysis of the X-ray powder diffraction patterns, we show that the increase in the concentration of Pb²⁺ and Sr²⁺ doping results in the structural transition from La₄Ti₉O₂₄ to a La_2/3TiO₃-type phase (Ibmm, No. 74). A change in the crystalline phase considerably affects the microwave dielectric properties, increasing the ɛ_r from 37 to 130, reducing Q × f from 25,000 to 5500, and increasing temperature coefficient of the resonant frequency (TCF) from 15 to 300 ppm/°C.     

Low-temperature sintering and microwave dielectric properties of CaTi1−x(Fe0.5Nb0.5)xO3 ceramics with B2O3 addition

CaTi_1−x(Fe_0.5Nb_0.5)_xO₃ (0 ≤ x ≤ 1) dielectrics were synthesized via the solid state reaction route and structure analysis was performed together with the dielectric characterization. The substitution of Ti⁴⁺ by Fe³⁺/Nb⁵⁺ and developed phase were studied by X-ray diffraction. The dielectric constant and temperature coefficient of resonant frequency decrease rapidly with an increase of x. The influence of 1–5 wt.% B₂O₃ as a sintering additive investigated at CaTi_0.5(Fe_0.5Nb_0.5)_0.5O₃ solid solutions. The dielectric properties were found to strongly depend on the sintering conditions and contents of B₂O₃ additions. ɛ_r = 52.3, Q × f_o = 2930 GHz and T_f = 13 ppm/°C were obtained for CaTi_0.5(Fe_0.5Nb_0.5)_0.5O₃ specimen 3 wt.% B₂O₃ sintered at 900 °C for 2 h.     

Microwave dielectric properties of BaO–TeO2 binary compounds

A series of BaO–TeO₂ binary ceramic compounds were explored for microwave dielectric applications with ultra-low processing temperatures. During the calcination of mixed BaCO₃ and TeO₂ raw powders, BaTe₄O₉, BaTe₂O₆, BaTeO₃, and Ba₂TeO₅ phases were obtained through the sequential phase formations from Te-rich to Ba-rich phases at temperatures ranging from 500 to 850 °C. Sintering temperatures were as low as only 550 °C for the Te-rich phases. Barium tellurate ceramics exhibited excellent microwave dielectric properties with intermediate dielectric permittivities and high quality factors (Q). The dielectric properties at microwave frequencies were ε_r = 10–21, Q × f = 34,000–55,000 GHz, and TCf = − 51 to − 124 ppm/°C, depending on compositions.     

Microwave dielectric properties of Ba3La2Ti2Nb2−xTaxO15 ceramics

High dielectric constant and low loss ceramics in the system Ba₃La₂Ti₂Nb_2−xTa_xO₁₅ (x = 0–2) have been prepared by conventional solid-state ceramic route. Ba₃La₂Ti₂Nb_2−xTa_xO₁₅ solid solutions adopted A₅B₄O₁₅ cation-deficient hexagonal perovskite structure for all compositions. The materials were characterized at microwave frequencies. They show a linear variation of dielectric properties with the value of x. Their dielectric constant varies from 49.8 to 45.1, quality factor Q_u × f from 22,000 to 31,040 GHz and temperature variation of resonant frequency from + 6.9 to − 13.4 ppm/°C as the value of x increases. These low loss ceramics might be used for dielectric resonator (DR) applications.     

New dielectric materials of xSrTiO3–(1 − x)Ca(Mg1/3Nb2/3)O3 ceramic system at microwave frequency

The crystal structures and the microwave dielectric properties of the xSrTiO₃–(1 − x)Ca(Mg_1/3Nb_2/3)O₃ perovskite ceramic system have been investigated. In order to achieve a temperature-stable material, we studied a method of combining a positive temperature coefficient material with a negative one. SrTiO₃ has dielectric properties of dielectric constant ε_r ∼ 205, Q × f value ∼ 4200 GHz and a large positive τ_f value ∼ 1700 ppm/°C. Ca(Mg_1/3Nb_2/3)O₃ possesses high dielectric constant (ε_r ∼ 28), high quality factor (Q × f value ∼ 58,000 at 7 GHz) and negative τ_f value (− 48 ppm/°C). As the x value varies from 0.2 to 0.8, the xSrTiO₃–(1 − x)Ca(Mg_1/3Nb_2/3)O₃ system has the dielectric properties as follows: 40 < ε_r < 123, 4600 < Q × f < 33,400 and − 23 < τ_f < 600. A new microwave dielectric material, 0.3SrTiO₃–0.7Ca(Mg_1/3Nb_2/3)O₃, applicable in microwave devices is suggested and possesses the dielectric properties of a dielectric constant ε_r ∼ 46, a Q × f value ∼ 29,300 GHz (at 6.8 GHz) and a τ_f value ∼− 2 ppm/°C. A near-zero τ_f value can be achieved by adjusting the x value of xSrTiO₃–(1 − x)Ca(Mg_1/3Nb_2/3)O₃ ceramics.