Low-temperature sintering of (Zn0.8 Mg0.2)2SiO4-TiO2 ceramics

Effect of Li₂O-B₂O₃-SiO₂ (LBS) glass on the sintering behavior and the microwave dielectric properties of (Zn_0.8 Mg_0.2)₂SiO₄-TiO₂ (ZMST) ceramics were investigated. The Li₂O-B₂O₃-SiO₂ glass lowered the sintering temperature of ZMST ceramics effectively from 1250 to 870 °C. The unknown second phase, which was formed in the ZMST ceramics increased with the addition of LBS glass. With increasing the LBS glass content, the bulk density, dielectric constant (ε_r) and the maximum Q × f value decreased, and the temperature coefficient of resonant frequency (τ_f) shifted to a negative value. (Zn_0.8 Mg_0.2)₂SiO₄-TiO₂ ceramics with 3 wt.% Li₂O-B₂O₃-SiO₂ glass sintered at 870 °C for 2 h shows excellent dielectric properties: ε_r = 8.48, Q × f = 11500 GHz, and τ_f = 0 ppm/°C.     

Phase relations and microwave dielectric properties of vanadium modified Ba5Nb4O15 ceramics

Microwave dielectric ceramics of Ba₅Nb_4−xV_xO₁₅ (x = 0-1) were prepared by a solid-state reaction method. Vanadium substitution can markedly lower the sintering temperature of Ba₅Nb₄O₁₅ from 1450 to 1100 °C. The X-ray powder diffraction analysis reveals the multiphase nature of this system. A hexagonal-to-orthorhombic phase transition was also observed for the BaNb₂O₆ secondary phase. The microwave dielectric properties, such as τ_f, ε_r and Q × f value, decreased with increasing vanadium content for samples sintered at 1100 °C. There was an apparent increase in τ_f and Q × f value for samples (x ≥ 0.5) sintered at 1200 °C due to the hexagonal-to-orthorhombic phase transition of the BaNb₂O₆ phase. These results suggested that the microwave dielectric properties of multiphase ceramics strongly depended on the phase compositions and the phase transitions.     

Temperature stable high-Q microwave dielectric ceramics in (1 − x)BaTi4O9-xBaZn2Ti4O11 system

The microwave dielectric properties of (1 − x)BaTi₄O₉-xBaZn₂Ti₄O₁₁ ceramics were investigated by solid-state reaction technique for obtaining high-Q dielectric ceramics in BaO-ZnO-TiO₂ system. And they were strongly determined by the chemical composition. As x was increased from 0.05 to 0.50, BaZn₂Ti₄O₁₁ phase formed more and more. Therefore, the ε_r decreased from 37.3 to 32.8 and the Q × f values first raised from 45,300 GHz to 60,600 GHz (x = 0.30) and then started to decline to 58,700 GHz (x = 0.40), and the τ_f values varied gradually from 12 ppm/°C to − 13 ppm/°C. 0.7BaTi₄O₉-0.3BaZn₂Ti₄O₁₁ ceramics sintered at 1240 °C for 3 h had excellent comprehensive microwave dielectric properties: ε_r = 34.2, Q × f = 60,600 GHz and τ_f = − 2 ppm/°C.     

Microwave dielectric properties of Mg1.8Ti1.1O4 ceramics

Low-loss Mg_1.8Ti_1.1O₄ ceramics were prepared by the conventional solid-state route and their microwave dielectric properties were investigated for the first time. The forming of tetragonal-structured Mg_1.8Ti_1.1O₄ main phase associated with a second phase MgTiO₃ were confirmed by the X-ray diffraction patterns. However, the presence of the second phase would cause no significant variance in the dielectric properties of the specimen because the second phase properties are very similar to that of the main phase. A fine combination of microwave dielectric properties (?_r ∼ 15.74, Q × f ∼ 141,000 GHz at 10.57 GHz, τ_f ∼ − 52.4 ppm/°C) was achieved for Mg_1.8Ti_1.1O₄ ceramics sintered at 1450 °C for 4 h.     

Effects of Y2O3 addition on microwave dielectric characteristics of Al2O3 ceramics

Microwave dielectric characteristics of alumina ceramics with yttria addition were investigated. The sintering temperature was lowered, and the dielectric constant (ε_r) did not remarkably change by adding yttria. The microwave dielectric loss (tan δ) increased from 8.4 × 10^− 5 to 2.2 × 10^− 4, due to the presence of Al₅Y₃O₁₂ secondary phase. The grain size had significant effects on the dielectric loss, and there was an optimum grain size where the dielectric loss reached the minimum.     

Microwave dielectric properties of Ba2 − xSrxLa3Ti3NbO15 ceramics

High dielectric constant and low loss ceramics in the system Ba_2 − xSr_xLa₃Ti₃NbO₁₅ (x = 0-1) have been prepared by conventional solid-state ceramic route. Ba_2 − xSr_xLa₃Ti₃NbO₁₅ 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 48.34 to 43.03, quality factor Q_u × f from 20,291 to 39,088 GHz and temperature variation of resonant frequency from 8 to 1.39 ppm/°C as the value of x increases. These low loss ceramics might be used for dielectric resonator (DR) applications.     

Influence of ZnO additions to 0.8(Mg0.95Co0.05)TiO3–0.2Ca0.6La0.8/3TiO3 ceramics on sintering behavior and microwave dielectric properties

The effects of ZnO addition on the microstructures and microwave dielectric properties of 0.8(Mg_0.95Co_0.05)TiO3–0.2Ca_0.6La_0.8/3TiO₃ ceramics were investigated. ZnO was selected as liquid phase sintering aids to lower the sintering temperature of 0.8(Mg_0.95Co_0.05)TiO3–0.2Ca_0.6La_0.8/3TiO₃ ceramics. With ZnO additives, the densification temperature of 0.8(Mg_0.95Co_0.05)TiO₃–0.2Ca_0.6La_0.8/3TiO₃ can be effectively reduced from 1450 to 1200–1325 °C. The crystalline phase exhibited no phase difference at low addition levels (0.25–2 wt.%). It is found that low-level doping of ZnO (0.25–2 wt.%) can significantly improve the density and dielectric properties of 0.8(Mg_0.95Co_0.05)TiO₃–0.2Ca_0.6La_0.8/3TiO₃ ceramics. The quality factors Q × f were strongly dependent upon the amount of additives. Q × f values of 36 000 and 13 000 GHz could be obtained at 1200–1325 °C with 1 and 2 wt.% ZnO additives, respectively. During all additives ranges, the relative dielectric constants were significantly different and ranged from 23.1 to 27.96. The temperature coefficient varies from 14.1–24.3 ppm/°C.     

Elastic tensor of the forsterite (Mg2SiO4) under pressure

A complete elastic tensor of the low-pressure structure of the magnesium orthosilicate (Mg₂SiO₄, forsterite) is determined by an ab initio technique for the pressure range P=0–240 kB. The geologically important quantities: density, sound velocity, Young's modulus, Poisson's ratio, crystal anisotropy, are derived from the calculated data. A systematic increase of crystal's anisotropy with pressure has been noticed. The results agree well with the available experimental data.     

Structural and dielectric studies of Li2SiO3 ceramic

Lithium metasilicate (Li₂SiO₃) ceramic was prepared via solid-state reaction technique. X-ray diffraction pattern showed that Li₂SiO₃ ceramic is orthorhombic. Microstructural analysis by field emission scanning electron microscopy (FE-SEM) shows that the compound has well defined grains separated by grain boundaries. Dielectric studies of the compound shows a strong frequency dispersion of permittivity in the low frequency region followed by a nearly frequency independent behavior in the high frequency region. The dielectric permittivity and dielectric loss at 5 MHz are 25.66 and 0.033 at room temperature. The activation energy (E_a) of the sample calculated from the plot of ac conductivity versus inverse of absolute temperature was found to be less than 1 eV. The smaller activation energy of the compound within moderate temperature range suggests the presence of singly ionized oxygen vacancies in the conduction process.     

A new low-loss microwave dielectric using (Ca0.8Sr0.2)TiO3-doped MgTiO3 ceramics

The microwave dielectric properties and the microstructures of the (1-x)MgTiO₃-x(Ca_0.8Sr_0.2)TiO₃ ceramic system prepared by the conventional solid-state route were investigated. (Ca_0.8Sr_0.2)TiO₃ was employed as a τ_f compensator and was added to MgTiO₃ to achieve a temperature-stable material. Ilmenite-structured MgTiO₃ and perovskite-structured (Ca_0.8Sr_0.2)TiO₃ were coexisted and the two-phase system was confirmed by the X-ray diffraction patterns and the energy-dispersive X-ray analysis. Although the ε_r of the specimen could be boosted by increasing amount of (Ca_0.8Sr_0.2)TiO₃, it would instead render a decrease in the Q × f. The τ_f value is strongly correlated to the compositions and can be controlled through the existing phases. In fact, τ_f could be adjusted to a near-zero value by mixing 94 mole% MgTiO₃ and 6 mole% (Ca_0.8Sr_0.2)TiO₃. A dielectric constant (ε_r) of 21.42, a high Q × f value of 83,700 GHz (at 9 GHz) and a temperature coefficient of resonant frequency (τ_f) of − 1.8 ppm/°C were obtained for 0.94MgTiO₃-0.06(Ca_0.8Sr_0.2)TiO₃ sintered at 1300 °C for 4 h. It is proposed as a low-loss and low-cost dielectric material for microwave and millimeter wave applications.     

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.     

Effect of Na2W2O7 addition on low-temperature sintering and microwave dielectric properties of CaWO4

Effects of Na₂W₂O₇ addition on low-temperature sintering, microstructure and microwave dielectric properties of CaWO₄ were studied by X-ray diffraction (XRD), scanning electron microscopy (SEM) and microwave dielectric resonator methods in this paper. The CaWO₄ material could be sintered into a dense ceramic (~ 96% theoretical density) at 850 °C/2 h without affecting its microwave dielectric properties greatly by adding appropriate amount of Na₂W₂O₇. The XRD results showed that CaWO₄ main phase with trace amount of Na₂W₂O₇ second phase was observed in (1 − x) CaWO4-xNa₂W₂O₇ (0 < x ≤ 0.04) ceramics. The chemical compatibility of 0.96CaWO₄-0.04Na₂W₂O₇ ceramic with silver (Ag) powders was also investigated. The Ag showed inert behavior with 0.96CaWO₄-0.04Na₂W₂O₇ ceramic when co-fired at 875 °C for 2 h.     

ZrSiO4 ceramics for microwave integrated circuit applications

The sintering temperature of ZrSiO₄ ceramic was optimized by studying the variation of density as a function of temperature. The dielectric properties were investigated at the radio and microwave frequencies. It has ε_r = 10.5, tan δ = 0.0016 (at 1 MHz), ε_r = 7.4, tan δ = 0.0006 (at 5.15 GHz) and τ_ε = 225 ppm/°C (at 1 MHz). The ceramic exhibited a negative coefficient of thermal expansion (CTE) of − 2.4 ppm/°C in the temperature range of 30-800 °C.     

Synthesis of nanocrystalline forsterite (Mg2SiO4) powder by combined mechanical activation and thermal treatment

This study investigates the synthesis of single-phase nanocrystalline forsterite powder by mechanical activation with subsequent annealing. To produce forsterite powder, a mixture of talc and magnesium oxide powders was first milled by a planetary ball mill, and then annealed at 1000 and 1200 °C for 1 h. The synthesized powder was characterized by X-ray diffraction (XRD), simultaneous thermal analysis (STA), scanning electron microscopy (SEM), and atomic absorption spectrometry (AAS). The initial temperature of forsterite crystallization was reduced to about 825 °C after 20 h of mechanical activation. The forsterite powder synthesized by 5 h of mechanical activation with subsequent annealing at 1000 °C for 1 h had crystallites 40 nm in size. The particle size of this sample was less than 500 nm.     

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.     

Dielectric properties of Ba(Ti1 − xZrx)O3 solid solutions

This paper reports the structural and dielectric properties of Ba(Ti_1 − xZr_x)O₃ (x = 0-0.3) ceramics. Single-phase solid solutions of the samples were determined by X-ray diffraction. Microscopic observation by scanning electron microscope revealed dense, single-phase microstructure with large grains (20-60 μm). The evolution of dielectric behavior from a sharp ferroelectric peak (for x ≤ 0.08) to a round dielectric peak (for 0.15 ≤ x ≤ 0.25) with pinched phase transitions and successively to a ferroelectric relaxor (for x = 0.3) was observed with increasing Zr concentration. Compared with pure BaTiO₃, broaden dielectric peaks with high dielectric constant of 25,000-40,000 and reasonably low loss (tanδ: 0.01-0.06) in the Ba(Ti_1 − xZr_x)O₃ ceramics have been observed, indicating great application potential as a dielectric material.     

Microwave dielectric properties of alkaline earth orthosilicates M2SiO4 (M=Ba, Sr, Ca)

Alkaline earth orthosilicates M₂SiO₄ (M=Ba, Sr, Ca) ceramics were prepared by solid state ceramic route and their microwave dielectric properties were investigated. M₂SiO₄ ceramics have ε_r in the range 8.5-13. At microwave frequencies, the Q_u × f obtained were 17,900 GHz, 19,100 GHz and 26,100 GHz for Ba₂SiO₄, Sr₂SiO₄ and Ca₂SiO₄ respectively. The τ_f of Ba₂SiO₄ was − 17 ppm/°C, whereas Sr₂SiO₄ and Ca₂SiO₄ exhibited high values of τ_f, − 205 ppm/°C and − 89 ppm/°C respectively. The coefficient of thermal expansion (α_l) of the orthosilicates was also studied.     

Synthesis and dielectric characterization of Ba0.6Sr0.4TiO3 ferroelectric ceramics

Ferroelectric ceramics Ba_0.6Sr_0.4TiO₃ (BST 40) were prepared, by solid-state reaction in the temperature range 1210-1450 °C. Maximum values of the ceramic densities were around 94% of their theoretical value. X-ray diffraction techniques (XRD) and scanning electron spectroscopy (SEM) were used to analyze the structure and the surface morphology of ceramics. Rounded, well defined or abnormal granular growth was observed in the SEM images, vs. sintering conditions and purity of the raw materials. In all samples, BST 40 ceramic is the major phase, but there are also present small amounts of secondary phases, as revealed in XRD diffraction patterns. Permittivity and dielectric loss measurements were performed in the temperature range − 150 to + 150 °C, and 150 Hz-5 MHz frequency values. Permittivity values rising from 1200 to 12,500, with increasing sintering temperatures, were recorded. Narrow and well defined transition peaks were noticed at higher sintering temperatures. Curie temperature was around 2 °C, for samples with the mentioned composition. Permittivity and losses vs. frequency show different behavior whether BST ceramics are in polar or non-polar state and with the distance toward phase transition. Microwave measurements performed at room temperature have shown lower values of permittivity, compared with similar data at low frequency, and dielectric losses lower than 1% at 0.7 GHz. The sintering conditions (temperatures, sintering time, etc.) and purity of the raw materials lead to important changes of transition temperatures in the polymorphic diagram, which we have built—for the other Ba1−xSrxTiO3 compositions (x = 0.25-0.90) sintered at 1260 °C for 2 h.     

Microwave dielectric properties of Mg4Al2Ti9O25 ceramics

Phase-singular Mg₄Al₂Ti₉O₂₅ ceramics with the pseudobrookite structure suitable for microwave devices such as antenna substrate have been prepared by gel-carbonate method with the dielectric permittivity of 24.7 (at 2-8 GHz), Q-values > 30,000 and temperature coefficients in permittivity (TCK) of less than + 17 ppm K^− 1. The dielectric characteristics are accountable in terms of ordering in the cation sub-lattice.