Microstructure and thermal properties of dysprosium and thulium co-doped barium titanate ceramics for high performance multilayer ceramic capacitors

The co-doping characteristics on microstructure and thermal properties of barium titanate (BaTiO₃) were investigated to elucidate formation of core-shell structure by dysprosium (Dy) and thulium (Tm) addition in the BaTiO₃-Dy₂O₃-Tm₂O₃ system. The dielectrics co-doped with 0.7 mol% Dy₂O₃ and 0.3 mol% Tm₂O₃ had the dielectric constant up to 2200 as a function of temperature, which was 30% higher than that of specimen containing only Tm₂O₃ at the room temperature. It could be explained by the fact that the increase of Dy₂O₃ addition contributed to the improvement of dielectric constant. On the other hand, the rapid diffusion rate of Dy³⁺ ions in BaTiO₃ showed an adverse effect on temperature stability caused by destruction of core-shell. As the compensation for shell expansion in BaTiO₃, the reinforcement of the core-shell structure through the addition of Tm₂O₃ was confirmed by TEM-EDS analysis and attributed the temperature coefficient of capacitance (TCC) in a reliability condition (−55 °C to 125 °C, △C = ±15% or less). The enhanced electrical properties and temperature stability could be deduced from the generation of electrons and the formation core-shell structure in co-doped BaTiO₃ system respectively.     

Sintering and crystallization of cordierite glass ceramics for high frequency multilayer chip inductors

Cordierite-based ceramics were developed by sintering a glass selected from MgO-Al₂O₃-SiO₂ system with an aim to use the material as high frequency chip inductors. A small amount of B₂O₃ and P₂O₅ were added to optimize the preparation conditions. The glass powder and sintered bodies were characterized by different analytical techniques such as TG-DTA analysis, X-ray diffraction, transmission and scanning electron microscopy. Pellets uniaxially pressed from the glass power could be sintered well at 950 °C having a density of above 99% theoretically, dielectric constant of 5.5, dielectric loss of 0.001 and thermal expansion coefficient of 26.7×10⁻⁷ °C⁻¹ (20-400 °C). Crystalline phases in this sintered sample are predominantly α-cordierite (hexagonal high cordierite) and trace amount of μ-cordierite. SEM depicted a uniformly dense microstructure with crystals of granular habit in the sintered sample.     

Non-destructive detection and localization of defects in multilayer ceramic chip capacitors using electromechanical resonances

High reliability multilayer ceramic chip capacitors are necessary for use in surface mounting processes which are more mechanically and thermally severe than the traditional through-hole processes. Moreover, in specific environments, even a small defect can be considered as catastrophic for the working of the electronic circuit or even of the entire system. In order to look for the failures—intrinsic latent defects and those caused by SMT soldering processes—appearing in these components, many techniques of analysis can be used. With this present work, we focus on one technique based on the principle of electromechanical resonances existing in piezoelectric materials under a d.c. bias field. The free correlation between the impedance measurement of the chip under a sufficient voltage allows us to highlight some conclusions concerning the behaviour, the nature of the defects and the long-term reliability of ceramic chip capacitors. This method has the advantage of being non-destructive, rapid, efficient and low-cost.     

Enhanced dielectric,ferroelectric and optical properties of lead free (K0.17Na0.83)NbO3 ceramic with WO3 addition

Polycrystalline lead-free ceramics (K_0.17Na_0.83)NbO₃ + x wt.% WO₃; (x = 0, 1, 3 and 5) have been synthesized via solid state reaction method. X-ray diffraction pattern at room temperature indicates the formation of pure perovskite phase with monoclinic structure for all samples. Dielectric constant versus temperature measurements shows an increase in dielectric constant with a shift in Curie temperature (T_C) toward higher temperature side. Remnant polarization (P_r) is found to be enhanced and reached upto 24 μC/cm² for x = 5 wt.% WO₃ from 12.5 μC/cm² for pure (K_0.17Na_0.83)NbO₃ ceramic. The value of coercive field (E_c) decreases with increasing wt.% of WO₃. From optical band gap study, we found blue shift in the band gap of (K_0.17Na_0.83)NbO₃ with increasing concentration of WO₃.     

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.     

Sintering behavior and dielectric properties of Ce doped strontium barium niobate ceramics with silica sintering additive

Sr_0.5Ba_0.5Nb₂O₆ ceramics with and without CeO₂ dopant were prepared by a partial co-precipitation method and a liquid phase sintering process. The cooperative effects of Ce doping and silica sintering additive on the sintering behaviors and the dielectric properties of Sr_0.5Ba_0.5Nb₂O₆ ceramics was investigated. It was observed that the lattice parameters of a-axis and c-axis of Sr_0.5Ba_0.5Nb₂O₆ ceramics decrease with the increase of Ce dopant, namely contraction of crystal cell volume occurs. Amorphous silica used for sintering additive can effectively restrain abnormal grain growth and prevent the rise of sintering activation energies caused by Ce doping, but Ce doping has more effect on the average size of the grains and the dielectric properties than the silica sintering additive when the Ce dopant and the silica sintering additive are introduced. Both the Curie temperatures and the maximum of dielectric constant at Tc decrease as the Ce³⁺ concentration increases.     

A low-temperature reactive sintering process for the 5Li2O–1Nb2O5–5TiO2 microwave dielectric ceramics

The B₂O₃-doped 5Li₂O–1Nb₂O₅–5TiO₂ composite microwave dielectric ceramics prepared by conventional and low-temperature single-step reactive sintering processes were investigated in the study. Without any calcinations involved, the Nb₂O₅ mixture of Li₂CO₃ and TiO₂ was pressed and sintered directly in the reactive sintering process. More uniform and finer grains could be obtained in the 5Li₂O–1Nb₂O₅–5TiO₂ ceramics by reactive sintering process, which could effectively save energy and manufacturing cost. And relatively good microwave dielectric properties of _r = 41, Q × f = 9885 GHz and τ_f = 43.6 ppm/°C could be obtained for the 1 wt.% B₂O₃-doped ceramics reactively sintered at 900 °C.     

Effect of CuO addition in Bi-Sr-Ca-Cu-O and Y-Ba-Cu-O ceramics

The effect of adding CuO matrix to Bi_1·6Pb_0·4Sr₂Ca₂Cu₃O_δ and Y₁Ba₂Cu₃O_δ superconductors was investigated through resistivity, XRD, SEM, thermoelectric power (TEP), and ac magnetization studies. Samples with as low as 20% (by weight) of the superconducting phase showed superconducting transition in resistivity-temperature (R-T), with the superconducting zero around 77 K in thermoelectric power, critical current (J _c) values were evaluated by applying Bean’s critical state model. CuO could be added to the superconducting material without any significant deterioration in the quality of the samples, up to a concentration of as low as 40% (by weight) of the superconducting material.     

Effect of A-site and B-site ion replaced with small ions on the intermediate phase in PbZrO3 ceramic

The solid solution of (1 − x)PbZrO₃–xNaNbO₃ ceramics, where x = 0.0–0.08, was synthesized by solid state reaction. The basic characterizations were performed using X-ray diffraction (XRD), dielectric spectroscopy, hysteresis measurement and differential scanning calorimetry (DSC) techniques. The results indicated that the crystal structure of the solid solution, (1 − x)PZ–xNN, where x = 0.00–0.08, is of orthorhombic symmetry. It was found that the effect of NN being replaced with small ions at the A-site and B-site can induce an AFE-like phase in PZ. The FE intermediate phase of PZ cannot be induced, although Zr⁴⁺ ions were substituted by small Nb⁵⁺ ions. This is due to the decreasing average rate of radii in the A-site (0.1 Å mol⁻¹) being higher than that in the B-site (0.08 Å mol⁻¹).     

Microstructural and piezoelectric properties of low temperature sintering PMN-PZT ceramics with the amount of Li2CO3 addition

PMN-PZT ceramics doped with Li₂CO₃ and Bi₂O₃ as sintering aids were manufactured in order to develop the low temperature sintering ceramics for multilayer piezoelectric transformer, and their micro structural, dielectric and piezoelectric properties were investigated. The sintering aids were proved to lower the sintering temperature of doped PMN-PZT ceramics due to the effect of LiBiO₂ liquid phase. Optimal values for multilayer piezoelectric transformer application, such as electromechanical coupling factor (k_p) of 0.50, mechanical quality factor (Q_m) of 2264, and dielectric constant (K) of 1216, and curie temperature (T_c) of 317 °C were found at 0.1 wt.% Li₂CO₃ added ceramics sintered at 940 °C.     

Microwave dielectric properties and microstructures of MgTa2O6 ceramics with CuO addition

The effect of CuO addition on the microstructures and the microwave dielectric properties of MgTa₂O₆ ceramics has been investigated. It is found that low level-doping of CuO (up to 1 wt.%) can significantly improve the density of the specimens and their microwave dielectric properties. Tremendous sintering temperature reduction can be achieved due to the liquid phase effect of CuO addition observed by scanning electronic microscopy (SEM). The sintered samples exhibit excellent microwave dielectric properties, which depend upon the liquid phase and the sintering temperature. With 0.5 wt.% CuO addition, MgTa₂O₆ ceramic can be sintered at 1400 °C and possesses a dielectric constant (_r) of 28, a Q × f value of 58000 GHz and a temperature coefficient of resonant frequency (τ_f) of 18 ppm/°C.     

Enhanced characteristics of Ba5SmTi3Nb7O30 ferroelectric nanocrystalline ceramic prepared by mechanical activation process: A comparative study

In the present work, structural, dielectric, ferroelectric, piezoelectric and pyroelectric properties of tungsten-bronze structured Ba₅SmTi₃Nb₇O₃₀ ceramics, synthesized by mechanical activation and conventional solid-state reaction processes, have been studied with an objective of comparing the properties of the specimens synthesized by the two processes. X-ray diffraction analysis shows the formation of the compound in an orthorhombic structure by both the processes. Scanning electron microscopy reveals the formation of a fine granular microstructure in the specimen synthesized by mechanical activation process compared to the specimen synthesized by conventional solid-state method. The specimen prepared using mechanical activation process exhibits improved electrical properties with higher dielectric constant, lower dielectric loss and higher resistivity. The effective remanent polarization () value, d₃₃ value and pyroelectric coefficients are also observed to be higher in the sample synthesized by the mechanical activation process.     

Sintering and dielectric properties of 0.88Al2O3-0.12TiO2 microwave ceramics by glass addition

The microwave characteristics and the microstructures of 0.88Al₂O₃-0.12TiO₂ with various amounts of MgO-CaO-SiO₂-Al₂O₃ (MCAS) glass sintered at different temperatures have been investigated. The sintering temperature can be lowered to 1300 °C by the addition of MCAS glass. The densities, dielectric constants (ε_r) and quality values (Q×f) of the MCAS-added 0.88Al₂O₃-0.12TiO₂ ceramics decrease with the increase of MCAS glass content. The temperature coefficients of the resonant frequency (τ_f) are shifted to more negative values as the MCAS content or the sintering temperatures increase. The change of the crystalline phases of Al₂TiO₅ phase and rutile-TiO₂ phase has profound effects on the microwave dielectric properties of the MCAS-added Al₂O₃-TiO₂ ceramics. As sintered at 1250 °C, 0.88Al₂O₃-0.12TiO₂ ceramics with 2 wt.% MCAS glass addition exists a ε_r value of 8.63, a Q×f value of 9578 and a τ_f value of +5 ppm/°C.     

Effects of grain boundary on dielectric properties in fine-grained BaTiO3 ceramics

BaTiO₃ dielectric ceramics, which have no core–shell structure, were prepared. High-resolution transmission electron microscope (TEM) and the newly developed chemical etching analysis revealed the composition of the grain boundary. The grain boundary has an important role in stabilizing temperature dependence of a dielectric constant. The grain boundary causes a large stress against grains, resulting in a change of the domain structure. So, the stress from the grain boundary is considered to depress the dielectric abnormality at the Curie temperature.     

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.     

Phase evolution and dielectric properties of MgTi2O5 ceramic sintered with lithium borosilicate glass

Phase evolution, densification, and dielectric properties of MgTi₂O₅ dielectric ceramic, sintered with lithium borosilicate (LBS) glass, were studied. Reaction between LBS glass and MgTi₂O₅ was significant in forming secondary phases such as TiO₂ and (Mg,Ti)₂(BO₃)O. The glass addition was not necessarily deleterious to the dielectric properties due to the formation of TiO₂: permittivity increased and temperature coefficient of resonance frequency could be tuned to zero with the addition of LBS glass, although the inevitable glass-induced decrease of quality factor was not retarded by the formation of TiO₂. The sintered specimen with 10 wt% LBS fired at 950 °C for 2 h showed permittivity of 19.3, quality factor of 6800 GHz, and τ_f of −16 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 glass fillers in Cu2ZnNb2O8 ceramics for advanced microwave applications

The effect of glass addition on sintering temperature and microwave dielectric properties of Cu₂ZnNb₂O₈ (CZN) is investigated for possible low temperature co-fired ceramic (LTCC) application. The CZN ceramic was prepared by the solid-state ceramic route. The phase formation, microstructure and elemental composition of the ceramics were studied using X-Ray Diffraction, Scanning Electron Microscopy, Transmission Electron Microscopy and Energy Dispersive Analysis. The CZN sintered at 975 °C/4 h has ?_r = 15.2, tan δ = 0.0007 (at 5.1 GHz) and τ_f of −98 ppm °C⁻¹ and CTE = 1.9 ppm °C⁻¹. The addition of LBS and LMZBS glasses lowered the sintering temperature of CZN to below the melting point of silver. The 1 wt% LBS added CZN sintered at 935 °C/4 h had ?_r = 14.7, tan δ = 0.001 (at 5.1 GHz), τ_f = −19 ppm °C⁻¹ and CTE = −0.6 ppm °C⁻¹. The addition of 0.7 wt% LMZBS to CZN and sintered at 935 °C/4 h had ?_r = 14.8, tan δ = 0.002 (at 5.1 GHz), τ_f = −39 ppm °C⁻¹ and CTE = −0.9 ppm °C⁻¹.     

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.     

Coupling of conductivity to the relaxation process in polymer electrolytes

Conductivity relaxation using modulus formalism has been used to explore the coupling of ionic conductivity to dielectric relaxation in polymer electrolyte based on polyethylene oxide complexed with various content of LiAsF₆. The temperature dependence of conductivity followed the VTF behavior suggesting close correlation between conductivity and the segmental relaxation process in polymer electrolytes. The coupling of conductivity to the segmental process has been discussed in terms of coupling index. For all compositions studied, the coupling index was within the range of 1–11 in the temperature range of investigation, which was in agreement with the coupled systems.