Low-firable high-K dielectric in the Zrx(Zn1/3Nb2/3)1−xTiO4 ceramic system

Composite ceramics in the solid solution of Zr_x(Zn_1/3Nb_2/3)_1−xTiO₄ (x = 0.1-0.4) have been prepared by the mixed oxide route. Formation of solid solution was confirmed by the X-ray diffraction patterns. The microwave dielectric properties, such as dielectric constant (?_r), Q × f value and temperature coefficient of resonant frequency (τ_f) have been investigated as a function of composition and sintering temperature. With x increasing from 0.1 to 0.4, the dielectric constant decreases from 70.9 to 43.2, and the τ_f decreases from 105 to 55 ppm/°C. The Q × f value, however, increases with increasing x value to a maximum 26,600 GHz (at 6 GHz) at x = 0.3, and then decreases thereafter. For low-loss microwave applications, a new microwave dielectric material Zr_0.3(Zn_1/3Nb_2/3)_0.7TiO₄, possessing a fine combination of microwave dielectric properties with a high ?_r of 51, a high Q × f of 26,600 GHz (at 6 GHz) and a τ_f of 70 ppm/°C, is suggested.     

Crystal structure and dielectric properties of La(Mg1−xZnx)1/2Ti1/2O3 ceramics at microwave frequencies

Ceramics in the system La(Mg_1−xZn_x)_1/2Ti_1/2O₃ with B₂O₃ additions (1 wt.%) have been investigated by the conventional solid-state route. The XRD patterns of the sintered samples (0.3 ≤ x ≤ 1.0) revealed single phase formation with a structure. The unit cell volume slightly increased with increasing Zn content (x). La(Mg_1−xZn_x)_1/2Ti_1/2O₃ were found to form perovskite solid solutions in the whole compositional range. The maximum values of the dielectric constant and the quality factor multiples resonant frequency (Q × f) can be obtained when the La(Mg_0.7Zn_0.3)_1/2Ti_1/2O₃ with 0.5 wt.% B₂O₃ additive were sintered at 1475 °C for 4 h. The temperature coefficient of resonant frequency τ_f (−63 ppm/°C) was measured for x = 0.7.     

High-dielectric-constant and low-loss microwave dielectric in the (1 − x)La(Mg0.5Ti0.5)O3-x(Ca0.8Sr0.2)TiO3 solid solution system

The microwave dielectric properties and microstructures of (1 − x)La(Mg_0.5Ti_0.5)O₃-x(Ca_0.8Sr_0.2)TiO₃ ceramics, prepared by a mixed oxide route, have been investigated. The forming of solid solutions was confirmed by the XRD patterns and the measured lattice parameters for all compositions. A near zero τ_f was achieved for samples with x = 0.5, although the dielectric properties varied with sintering temperature. The Q × f value of 0.5La(Mg_0.5Ti_0.5)O₃-0.5(Ca_0.8Sr_0.2)TiO₃ increased up to 1475 °C, after which it decreased. The decrease in dielectric properties was coincident with the onset of rapid grain growth. The optimum combination of microwave dielectric properties was achieved at 1475 °C for samples where x = 0.5 with a dielectric constant ?_r of 47.12, a Q × f value of 35,000 GHz (measured at 6.2 GHz) and a τ_f value of −4.7 ppm/°C.     

Structure and dielectric characterization of xNd(Mg1/2Ti1/2)O3-(1 − x)Ca0.6La0.8/3TiO3 in the microwave frequency range

The crystal structures, phase compositions and the microwave dielectric properties of the xLa(Mg_1/2Ti_1/2)O₃-(1 − x)Ca_0.8Sr_0.2TiO₃ composites prepared by the conventional solid state route have been investigated. The formation of solid solution is confirmed by the XRD patterns. Doping with B₂O₃ (0.5 wt.%) can effectively promote the densification and the dielectric properties of xNd(Mg_1/2Ti_1/2)O₃-(1 − x)Ca_0.6La_0.8/3TiO₃ ceramics. It is found that xNd(Mg_1/2Ti_1/2)O₃-(1 − x)Ca_0.6La_0.8/3TiO₃ ceramics can be sintered at 1375 °C, due to the liquid phase effect of B₂O₃ addition observed by Scanning Electronic Microscopy. At 1375 °C, 0.4Nd(Mg_1/2Ti_1/2)O₃-0.6Ca_0.6La_0.8/3TiO₃ ceramics with 1 wt.% B₂O₃ addition possesses a dielectric constant (?_r) of 49, a Q × f value of 13,000 (at 8 GHz) and a temperature coefficients of resonant frequency (τ_f) of 1 ppm/°C. As the content of Nd(Mg_1/2Ti_1/2)O₃ increases, the highest Q × f value of 20,000 GHz for x = 0.9 is achieved at the sintering temperature 1400 °C.     

Phase evolution, crystal structure and dielectric behavior of (1 − x)Nd(Zn0.5Ti0.5)O3 + xBi(Zn0.5Ti0.5)O3 compound ceramics

The phase evolution, crystal structure and dielectric properties of (1 − x)Nd(Zn_0.5Ti_0.5)O₃ + xBi(Zn_0.5Ti_0.5)O₃ compound ceramics (0 ≤ x ≤ 1.0, abbreviated as (1 − x)NZT-xBZT hereafter) were investigated. A pure perovskite phase was formed in the composition range of 0 ≤ x ≤ 0.05. The B-site Zn²⁺/Ti⁴⁺ 1:1 long range ordering (LRO) structure was detected by both XRD and Raman spectra in x ≤ 0.05 samples. However, this LRO structure became gradually degraded with an increase in x. The dielectric behaviors of the compound ceramic at various frequencies were investigated and correlated to its chemical composition and crystal structure. A gradually compensated τ_f value was obtained in (1 − x)NZT-xBZT microwave dielectrics at x = 0.03, which was mainly due to the dilution of dielectric constant in terms of Claussius-Mossotti differential equation.     

Microwave dielectric properties of (1 − x)ZnMoO4-xTiO2 composite ceramics

(1 − x)ZnMoO₄-xTiO₂ (x = 0.0, 0.05, 0.158, 0.25, and 0.35) composite ceramics were synthesized by the conventional solid state reaction process. The sintering behavior, phase composition, chemical compatibility with silver, and microwave dielectric properties were investigated. All the specimens can be well densified below 950 °C. From the X-ray diffraction analysis, it indicates that the triclinic wolframite ZnMoO₄ phase coexists with the tetragonal rutile TiO₂ phase, and it is easy for silver to react with ZnMoO₄ to form Ag₂Zn₂(MoO₄)₃ phase and hard to react with TiO₂. When the volume fraction of TiO₂ (x value) increasing from 0 to 0.35, the microwave dielectric permittivity of the (1 − x)ZnMoO₄-xTiO₂ composite ceramics increases from 8.0 to 25.2, the Q_f value changes in the range of 32,300-43,300 GHz, and the temperature coefficient τ_f value varies from −128.9 to 157.4 ppm/°C. At x = 0.158, the mixture exhibits good microwave dielectric properties with a ?_r = 13.9, a Q_f = 40,400 GHz, and a τ_f = +2.0 ppm/°C.     

Microwave dielectric properties of temperature stable Li2ZnxCo1−xTi3O8 ceramics

The Li₂Zn_xCo_1−xTi₃O₈ (x = 0.2-0.8) solid solution system has been synthesized by the conventional solid-state ceramic route and the effect of Zn substitution for Co on microwave dielectric properties of Li₂CoTi₃O₈ ceramics has also been investigated. The microwave dielectric properties of these ceramics show a linear variation between the end members for all compositions. The optimized sintering temperatures of Li₂Zn_xCo_1−xTi₃O₈ ceramics increase with increasing content of Zn. The specimen with x = 0.4 sintered at 1050 °C/2 h exhibits an excellent combination of microwave dielectric properties with ?_r = 27.7, Q_u × f = 57,100 GHz and τ_f = −1.0 ppm/°C.     

Synthesis, structural and microwave dielectric properties of Al2W3−xMoxO12 (x = 0-3) ceramics

Low dielectric ceramics in the Al₂W_3−xMo_xO₁₂ (x = 0-3) system have been prepared through solid state ceramic route. The phase purity of the ceramic compositions has been studied using powder X-ray diffraction (XRD) studies. The microstructure of the sintered ceramics was evaluated by Scanning Electron Microscopy (SEM). The crystal structure of the ceramic compositions as a result of Mo substitution has been studied using Laser Raman spectroscopy. The microwave dielectric properties of the ceramics were studied by Hakki and Coleman post resonator and cavity perturbation techniques. Al₂Mo_xW_3−xO₁₂ (x = 0-3) ceramics exhibited low dielectric constant and relatively high unloaded quality factor. The temperature coefficient of resonant frequency of the compositions is found to be in the range −41 to −72 ppm/°C.     

Microwave dielectric properties of (Zn1−xMgx)TiO3 (ZMT) ceramics for dielectric resonator antenna application

Present investigation provides experimental studies on cylindrical dielectric resonator antennas (CDRAs) fabricated from (Zn_1−xMg_x)TiO₃ (ZMT) ceramic material with different substitution of Mg in place of Zn (x = 0.1, 0.2, 0.3, 0.4 and 0.5) along with measurement of material permittivity in C-band of microwave frequencies. The dielectric properties of the ZMT ceramic materials with different x values (x = 0.1-0.5) have been measured at microwave frequencies using Hakki-Coleman method modified by Courtney. The value of dielectric constant and loss tangent decreases with the increase in Mg content. The dielectric constant is minimum for x = 0.3 and loss tangent is minimum for x = 0.5. The variations of return loss and input impedance versus frequency and radiation patterns of CDRAs at their respective resonant frequencies are studied experimentally. The measured results for resonant frequency and return loss bandwidth of the CDRAs are also compared with theoretical ones. The measured resonant frequencies of all the four CDRAs are nearly in agreement with respective theoretical values and the values of input resistance at respective resonant frequencies of the CDRAs match well with the coaxial feed impedance of 50 Ω. The designed CDRAs have broad beam, low side lobe and cross-polarized lobe levels.     

Enhancement microwave dielectric properties of La(Mg0.5Sn0.5)O3 ceramics by substituting Mg with Ni

The microwave dielectric properties of La(Mg_0.5−xNi_xSn_0.5)O₃ ceramics were examined with a view to their exploitation for mobile communication. The La(Mg_0.5−xNi_xSn_0.5)O₃ ceramics were prepared by the conventional solid-state method at various sintering temperatures. The X-ray diffraction patterns of the La(Mg_0.4Ni_0.1Sn_0.5)O₃ ceramics revealed no significant variation of phase with sintering temperatures. Apparent density of 6.71 g/cm³, dielectric constant (?_r) of 20.19, quality factor (Q × f) of 74,600 GHz, and temperature coefficient of resonant frequency (τ_f) of −85 ppm/°C were obtained for La(Mg_0.4Ni_0.1Sn_0.5)O₃ ceramics that were sintered at 1550 °C for 4 h.     

Dielectric properties and crystal structure of La(Mg1/2Ti1/2)O3 ceramics with Mg substituted by Co

Solid solutions of (1 − x)La(Co_1/2Ti_1/2)O₃-xLa(Mg_1/2Ti_1/2)O₃ were used to prepare La(Mg_1−xCo_x)_1/2Ti_1/2O₃ using solid-state synthesis. X-ray diffraction patterns of the sintered samples revealed single phase formation. A maximum density of 6.01 g/cm³ was obtained for La(Mg_1−xCo_x)_1/2Ti_1/2O₃ (x = 1) ceramics sintered at 1375 °C for 4 h. The maximum values of the dielectric constant (?_r = 29.13) and the quality factor (Q × f = 80,000 GHz) were obtained for La(Mg_1−xCo_x)_1/2Ti_1/2O₃ with 1 wt% ZnO additive sintered at 1375 °C for 4 h. The temperature coefficient of resonant frequency τ_f was −59 ppm/°C for x = 0.3.     

Low temperature sintering and microwave dielectric properties of (Mg0.7Zn0.3)0.95Co0.05TiO3 ceramics with BaCu(B2O5) additions

The effects of BaCu(B₂O₅) additives on the sintering temperature and microwave dielectric properties of (Mg_0.7Zn_0.3)_0.95Co_0.05TiO₃ ceramics were investigated. The (Mg_0.7Zn_0.3)_0.95Co_0.05TiO₃ ceramics were not able to be sintered below 1000 °C. However, when BaCu(B₂O₅) were added, they were sintered below 1000 °C and had the good microwave dielectric properties. It was suggested that a liquid phase with the composition of BaCu(B₂O₅) was formed during the sintering and assisted the densification of the (Mg_0.7Zn_0.3)_0.95Co_0.05TiO₃ ceramics at low temperature. BaCu(B₂O₅) powders were produced and used to reduce the sintering temperature of the (Mg_0.7Zn_0.3)_0.95Co_0.05TiO₃ ceramics. Good microwave dielectric properties of Q × f = 35,000 GHz, ?_r = 18.5.0 and τ_f = −51 ppm/°C were obtained for the (Mg_0.7Zn_0.3)_0.95Co_0.05TiO₃ ceramics containing 7 wt.% mol% BaCu(B₂O₅) sintered at 950 °C for 4 h.     

Crystal structure and microwave dielectric properties of ZnTi(Nb1−xTax)2O8 ceramics

The crystal structure and microwave dielectric properties of ZnTi(Nb_1−xTa_x)₂O₈ (0 ≤ x ≤ 1) ceramics sintered at 1200 °C for 2 h were investigated. For x < 0.5, solid solution phases with the α-PbO₂ structure, typical of ZnTiNb₂O₈, were obtained, whereas for 0.5 ≤ x < 1, mixtures of two solid solutions each respectively based on the α-PbO₂ structure and a trirutile structure, were obtained. The relative amount of the trirutile-structured phases increased as the Ta content increased in a given region, and the end member ZnTiTa₂O₈ formed a single phase with the trirutile structure. The microwave dielectric properties were closely related to the crystal structures. A material with a near zero temperature coefficient of resonant frequency could be obtained for x = 0.8, and its dielectric constant and quality factor (Q × f) were 40.5 and 41,000 GHz, respectively.     

Phase evolution and microwave dielectric properties of TiO2-modified (Mg0.95Co0.05)2TiO4 ceramics

Phase evolution and microwave dielectric properties of (1 − x)(Mg_0.95Co_0.05)₂TiO₄-xTiO₂ (x = 0-1) ceramics prepared by the conventional mixed oxide route have been investigated. Increasing the TiO₂ content would lead to a main phase transformation from (Mg_0.95Co_0.05)₂TiO₄ to (Mg_0.95Co_0.05)TiO₃, (Mg_0.95Co_0.05)Ti₂O₅ and then TiO₂. Not only did the TiO₂ addition compensate the τ_f, it also lowered the sintering temperature of specimen. A huge drop of Q × f occurs at a 40-60 mol% TiO₂ addition was attributed to the formation of (Mg_0.95Co_0.05)Ti₂O₅ phase. Specimen with x = 0.78 can possess an excellent combination of microwave dielectric properties: ?_r ∼ 24.77, Q × f ∼ 38,500 GHz and τ_f ∼ −1.3 ppm/°C.     

Effect of CaTiO3 addition on microwave dielectric properties of Mg2(Ti0.95Sn0.05)O4 ceramics

The microwave dielectric properties of CaTiO₃-added Mg₂(Ti_0.95Sn_0.05)O₄ ceramics prepared by the mixed oxide route have been investigated. The combination of spinel-structured Mg₂(Ti_0.95Sn_0.05)O₄ and perovskite-structured CaTiO₃ forms a two-phase system (1 − x)Mg₂(Ti_0.95Sn_0.05)O₄-xCaTiO₃, which was confirmed by the XRD patterns and the EDX analysis and it also leads to a zero τ_f. The microwave dielectric properties of the ceramics can be effectively controlled by varying the x value. For practical applications, a new microwave dielectric material 0.91Mg₂(Ti_0.95Sn_0.05)O₄-0.09CaTiO₃ is suggested and it possesses a good combination of dielectric properties with an ?_r of ∼18.01, a Q × f of ∼92,000 GHz, and a τ_f of ∼0 ppm/°C, which makes it is a very promising candidate material for high frequency applications.     

Dielectric properties of Cu substituted Ni0.5−xZn0.3Mg0.2Fe2O4 ferrites

Dielectric properties of Cu substituted Ni-Zn-Mg ferrite samples having the general formula Ni_0.5−xCu_xZn_0.3Mg_0.2Fe₂O₄ (where x = 0.0, 0.1, 0.2, 0.3, 0.4, and 0.5) synthesized by Pramanik method are reported. The single phase formation of the ferrites was confirmed by XRD technique. The lattice parameter is found to increase with increase in Cu content. Average grain size, obtained from SEM micrographs, is found to increase with increase in Cu content. Dielectric parameters were measured as a function of frequency at room temperature as well as at higher temperatures. The variation in dielectric constant (?′) with temperature at four different fixed frequencies viz. 1 kHz, 10 kHz, 100 kHz, and 1 MHz was also studied. The room temperature dielectric constant (?′) and dielectric loss (tan δ) are found to decrease with increase in frequency. The ac conductivity (σ_ac) is found to increase with increase in the frequency.     

Relationships between Zr substitution for Ti and microwave dielectric properties in Mg(ZrxTi1−x)O3 ceramics

The influence of Zr substitution for Ti on the microwave dielectric properties and microstructures of the Mg(Zr_xTi_1−x)O₃(MZ_xT) (0.01 ≤ x ≤ 0.3) ceramics was investigated. The quality factors of Mg(Zr_xTi_1−x)O₃ ceramics with x = 0.01-0.05 were improved because the solid solution of a small amount of Zr⁴⁺ substitution in the B-site could increase density and grain size. An excess of Zr⁴⁺ resulted in the formation of a great deal of secondary phase that declined the microwave dielectric properties of MZ_xT ceramics. The temperature coefficient of resonant frequency (τ_f) of Mg(Zr_xTi_1−x)O₃ ceramics slightly increased with increasing Zr content, and the variation in τ_f was attributed to the formation of secondary phases.     

Structural and microwave absorption properties of Ni(1−x)Co(x)Fe2O4 (0.0 ≤ x ≤ 0.5) nanoferrites synthesized via co-precipitation route

Ni-Co nanoferrites show excellent magneto-dielectric properties and these materials can be used to miniaturize the size of the high frequency devices which is the order of the day. Nanocrystalline Ni-Co ferrites having general formula Ni_1−xCo_xFe₂O₄ (x = 0.0, 0.1, 0.2, 0.3, 0.4, and 0.5) were prepared by co-precipitation method. The structural morphology of the prepared samples was carried out using scanning electron microscopy. The results showed the spherical shaped nanoparticles varying in the range of 16-40 nm. The complex relative permittivity (?_r) and complex relative permeability (μ_r) were measured using vector network analyzer for all the samples in the frequency range of 1 MHz to 3 GHz. The variation of complex relative permittivity (?_r) as a function of frequency is explained in accordance with Maxwell-Wagner model and Koop's phenomenological theory. The effect of frequency and cobalt concentration on permeability are reported. The reflectivity (R) of nanoferrites is also calculated. The value of minimum reflection loss (RL) is about −18 dB at 2.45 GHz with a thickness of 2.1 ± 0.1 mm. The results indicate that Ni_1−xCo_xFe₂O₄ nanoparticles have excellent microwave absorbing properties and have a great potential for military use.     

Preparation and characterization of La1−xKxFeO3 (x = 0-1) by self-propagating high-temperature synthesis for use as soot combustion catalyst

This paper proposes La_1−xK_xFeO₃ prepared by self-propagating high-temperature synthesis (SHS) as an alternative to platinum catalysts for promoting diesel soot combustion. The catalytic property of eleven products SHSed with different substitution ratios of potassium (x = 0-1) was experimentally evaluated using a thermobalance. In the mass loss curves of the product, T₅₀ was defined as the temperature at which the weight of the reference soot decreases to half its initial weight. The BET specific surface area of SHSed La_1−xK_xFeO₃ depended on x strongly. All the products showed good oxidation catalytic activity. Despite having the smallest surface area (0.11 m²/g) among the obtained products, La_0.9K_0.1FeO₃ (x = 0.1) was found to be the best catalyst with the lowest T₅₀ (442 °C). T₅₀ of La_1−xK_xFeO₃ decreased with increasing x for x > 0.2. The products with x = 0.6 and 0.8 were the second-best catalysts in terms of their T₅₀. Moreover, average apparent activation energy of La_0.9K_0.1FeO₃ (x = 0.1) calculated by Friedman method using TG was as much as 61 kJ/mol lower than that of Pt/Al₂O₃ catalyst. In conclusion, potassium-substituted SHSed La_1−xK_xFeO₃ can be used as an alternative to Pt/Al₂O₃ for soot combustion.     

Fabrication and properties of Ba(Zr1−xCex)0.9Y0.1O2.95/NaCl composite electrolyte materials

Ba(Zr_1−xCe_x)_0.9Y_0.1O_2.95/NaCl (x = 0.1, 0.2 and 0.3) composite electrolyte materials were fabricated with ZnO as sintering aid. The effect of ZnO on the properties of Ba(Zr_1−xCe_x)_0.9Y_0.1O_2.95 matrix were investigated. The phase composition and microstructure of samples were characterized by XRD and SEM, respectively. The electrochemical performances were studied by three-probe conductivity measurement and AC impedance spectroscopy. XRD results showed that Ba(Zr_1−xCe_x)_0.9Y_0.1O_2.95 with 2 mol% of ZnO was perovskite structure. The relative density of this sample was above 95% when sintered at 1450 °C for 6 h. By adding 10 mol% of NaCl to Ba(Zr_1−xCe_x)_0.9Y_0.1O_2.95 with 2 mol% of ZnO that was sintered at 1400 °C for 6 h, the conductivity was increased. The electrical conductivity of 1.26 × 10⁻² S/cm and activation energy of 0.23 eV were obtained when tested at 800 °C in wet hydrogen.