Influence of TiO2 additive on sintering temperature and microwave dielectric properties of Mg0.90Ni0.1SiO3 ceramics

(1-x)Mg_0.90Ni_0.1SiO₃-xTiO₂ (x = 0, 0.01, 0.03, 0.05) ceramics were successfully formed by the conventional solid-state methods and characterized by x-ray diffraction (XRD), scanning electron microscopy (SEM), and energy dispersive spectroscopy (EDS), and their microstructure and microwave dielectric properties systematically investigated. It was observed that when TiO₂ content increased from 0 to 5 wt%, the Q_uf_o of the sample decreased from 118,702 GHz to 101,307 GHz and increases the τ_f value from −10 ppm/°C to +3.14 ppm/°C accompanied by a notable lowering in the sintering temperature (125 °C). A good combination of microwave dielectric properties (ε_r ∼ 8.29, Q_uf_o ∼ 101,307 GHz and τ_f ∼ −2.98 ppm/°C) were achieved for Mg_0.90Ni_0.1SiO₃ containing 3 wt% of TiO₂ sintered at 1300 °C for 9 h which make this material of possible interest for millimeter wave applications.     

Effects of Zn2+/Mg2+ ratio on dielectric properties of BaTiO3-based ceramics with excellent temperature stability: Experiments and the first-principle calculations

To satisfy the development of MLCC devices, the dielectric properties and temperature stability of ceramic materials urgently needs to be improved. In our work, the 0.9BaTiO₃-0.1Bi(Zn_xMg_0.5-xY_0.5)O_2.75 ceramics with x=0.0–0.5 are successfully prepared based on a traditional solid-state method. Meanwhile, the ceramic sample (core-shell structure) with x = 0.1 exhibits excellent dielectric properties and temperature stability (ε_r: 1207, tanδ: 0.009 and ε_r/ε₂₅ ≤±15% within ?80 to 200 °C), which satisfies the Electronic Industries Association (EIA) X9R (-55–150 °C, Δε_r/ε₂₅ ≤±15%) specification. In addition, the physical mechanism behind dielectric properties and temperature stability is systematic investigated based on experimental characterization and the first-principle calculations. The interface polarization is regarded as the primary cause affecting the dielectric properties, and has a close relationship with shell structure of ceramic samples. The lattice deformation of shell structure is caused by the introduction of heterovalent ions and non-equivalent substitution. Dielectric constant may be advance as content of Zn²⁺ ions increases due to the electronic enrichment around the zinc site in distorted lattice matrix. However, the weaken force between atom and electron results in the poor temperature stability.     

Sintering temperature effect on microstructure,electrical properties and temperature stability of MnO-modified KNN-based ceramics

Lead-free 0.955K_0.5Na_0.5NbO₃-0.045Bi_0.5Na_0.5ZrO₃?+?0.6%MnO (KNN-0.045BNZ?+?Mn0.6) ceramics have been prepared by a conventional solid-state sintering method in air. All the samples sintered at different temperatures possess a coexisting phase boundary (CPB) between rhombohedral (R) phase and tetragonal (T) phase. The increase of sintering temperature (T_s) increases the phase fraction of T phase in CPB region. Mn²⁺, Mn³⁺ and Mn⁴⁺ ions coexist in all the KNN-0.045BNZ?+?Mn0.6 ceramics sintered at 1110?°C to 1190?°C. High sintering temperature can induce a transformation from ${\mathrm{M}\mathrm{n}}_{\mathrm{N}\mathrm{b}}^{\text{'}\text{'}}$ defects to ${\mathrm{M}\mathrm{n}}_{\mathrm{N}\mathrm{b}}^{\text{'}}$ defects. The samples with fine grain show stable octahedral structure. The KNN-0.045BNZ?+?Mn0.6 ceramics with fine grain possess excellent temperature stability of $d_{33}^{*}$ due to the wide phase transition region. The increase of sintering temperature induces the (R-T) phase transition temperature to move to room temperature.     

A new approach to producing transparent ZnAl2O4 ceramics

A new approach to producing of transparent bulk ZnAl₂O₄ ceramics based on hot pressing of powders (1600 °С, 50 МPа) in presence of sintering additive ZnF₂ is described. Using this approach in the presence of 5 wt% of ZnF₂ transparent ZnAl₂O₄ ceramics was prepared with transparency range from 0.2 to 7.5 μm and with band gap of about 6.05 eV. The average grain size was about 33 μm and the transmittance at the wavelength of 550 nm was about 63%.     

Enhanced piezoelectric properties and temperature stability of Bi4Ti3O12-based Aurivillius ceramics via W/Nb substitution

Bi₄Ti₃O₁₂ (BIT), a typical Aurivillius ceramics with high Curie temperature (T_c ? 675 °C), has great potential for high temperature applications. This work provides an effective method of inducing structure distortion, relieving the tetragonal strain of the TiO₆ octahedron and decreasing the concentration of oxygen vacancies to improve the piezoelectricity and temperature stability of BIT ceramics. Bi₄Ti_2.98W_0.01Nb_0.01O₁₂ possesses an optimum piezoelectric coefficient (d₃₃) of 32 pC/N, a high T_c of 655 °C and a large resistivity of 3 × 10⁶ Ω·cm at 500 °C. The maximum d₃₃ reported here is approximately quadruple than that of pure BIT (?7 pC/N). Moreover, the d₃₃ of W/Nb co-doped BIT and the in-situ temperature stability of the compression-mode sensor present a highly stable characteristic in the range of 25–600 °C. These results imply that W/Nb-modified BIT ceramics is a promising candidate for application at high temperatures of up to 600 °C.     

Enhanced energy storage properties of Bi0.5Na0.5TiO3-based ceramics via regulating the doping content and sintering temperature

Eco-friendly lead-free energy-storage ceramics featuring high energy storage properties and ultra-high stability have been regarded to be one of the most potential materials in the field of energy storage. In this work, a new element system, (1-x)(0.6Bi_0.5Na_0.5TiO₃-0.4SrTiO₃)-xBi[Zn_2/3(Nb_0.5Ta_0.5)_1/3]O₃ ((1-x)BNST-xBZNT) lead-free ceramics, were synthesized via a conventional solid-state sintering technology. And the phase structure, microstructure and energy storage properties of the (1-x)BNST-xBZNT ceramics were comprehensively studied. After the introduction of BZNT, the average grain size of the materials is greatly decreased, thereby enhancing the dielectric breakdown strength (DBS). Additionally, the thermal stability of the ceramics is significantly improved via regulating the doping content and sintering temperature. Furthermore, the ferroelectric long-range order of the ceramics is decomposed into randomly-oriented polar nano-domains (PNRs) after introducing BZNT, leading to strong relaxor behavior and significantly reducing remanent polarization (P_r). As a result, even under a relatively low electric field of 139 kV/cm, the 0.98BNST-0.02BZNT ceramic sintered at 1150 °C possesses high values of energy storage efficiency (η) value of 92.78% and total energy storage density (W_tot) of 1.67 J/cm³ as well as remarkable thermal stability (25–175 °C), frequency stability (20–70 Hz) and fatigue resistant stability (10⁰-10⁵ cycles). This investigation provides a useful reference for developing advanced energy storage ceramics by regulating the doping content and sintering temperature.     

Effect of complex Si4++Mg2+ additive on sintering and properties of undoped YAG ceramics

The paper is devoted to studying of Si⁴⁺+Mg²⁺ complex additive for obtaining transparent YAG ceramics for laser applications. Ceramics were fabricated by reactive vacuum sintering of commercial Y₂O₃, Al₂O₃ powders taken in a stoichiometric mixture with TEOS and MgO as sintering aids. Microstructure and optical properties of YAG:Si⁴⁺,Mg²⁺ ceramics were investigated as a function of the Si⁴⁺/Mg²⁺ ratio. It was found that the influence of complex additive does not correspond to the direct superposition of known Si⁴⁺- and Mg²⁺-induced sintering mechanisms and involves interaction between Si⁴⁺ and Mg²⁺ ions during sintering. It was shown that C_Si/C_Mg> 1 provides more effective pore elimination and uniform microstructure when C_Si/C_Mg< 1 gives more intense inhibition of grain grown which may be important for scaling the size of ceramics.     

Transient liquid-phase sintering of AlN ceramics with CaF2 additive

Transient liquid-phase (TLP) sintering of CaF₂ additive on the densification behaviors and microstructural development of AlN ceramics are investigated. It is found that 1 wt% CaF₂ can effectively promote densification process. Increasing content of CaF₂ results in finer grain size and slower densification during intermediate sintering stage. XRD results show that grain-boundary phase of CaAl₄O₇ is formed at 1150 °C from reactions of AlN–CaF₂–Al₂O₃. With further temperature increasing, the grain-boundary phases of CA2 and CaAl₁₂O₁₈, which were formed from the reaction between CaF₂ and oxide layers, experienced transformations firstly into CaAl₄O₇ above 1600 °C and into CaAl₂O₄ at higher temperature. SEM and TEM results show that formed grain-boundary phases can evaporate from sintering bodies during further soaking, leaving clean grain boundaries. The efficiency of TLP sintering mechanism is further manifested by the preparation of transparent AlN ceramics with good combination properties.     

Enhanced dielectric loss of Mg doped Ba0.7Sr0.3TiO3 ceramics

The effect of MgO doping on the structural, microstructural and dielectric properties of Ba_0.7Sr_0.3TiO₃ (BST) ceramic from the point of view of its application in microwave tunable devices has been studied. All the samples crystallize into perovskite structure. There is significant reduction in the value of loss factor with the increase in Mg-level, the dielectric constant and tunability are also reduced with the increase in Mg-level. Interestingly, the Fig. of merit of the material is found to be enhanced with increase of Mg-doping. The observed dielectric properties are explained on the basis of defect chemistry involved when Mg is doped in Ba_0.7Sr_0.3TiO₃ ceramics. The effect of dc field on the dielectric constant and the dielectric breakdown strength of the paraelectric phase Mg doped BST ceramic samples are also studied.     

Tuning the microwave dielectric properties of Zn2SnO4 ceramics by adding Ca0.8Sr0.2TiO3

The influence of sintering temperature on the microwave dielectric properties and microstructure of the (1−y)Zn₂SnO₄–yCa_0.8Sr_0.2TiO₃ ceramic system were investigated with a view to their application in microwave devices. A (1−y)Zn₂SnO₄–yCa_0.8Sr_0.2TiO₃ ceramic system was prepared by the conventional solid-state method. The X-ray diffraction patterns of the 0.85Zn₂SnO₄–0.15Ca_0.8Sr_0.2TiO₃ ceramic system did not significantly vary with sintering temperature. A dielectric constant of 9.6, a quality factor (Q×f) of 15,900 GHz, and a temperature coefficient of resonant frequency of −4 ppm/°C were obtained when the 0.85Zn₂SnO₄–0.15Ca_0.8Sr_0.2TiO₃ ceramic system was sintered at 1175 °C for 4 h.     

Effect of annealing temperature on structural and magnetic properties of Co2TiO4 ceramics prepared by sol-gel method

In this paper, polycrystalline Co₂TiO₄ ceramics have been synthesized using a sol-gel process followed by annealing at different temperatures. The lattice size and the average grain size of the samples increases with rise in annealing temperature. The temperature-dependent inverse paramagnetic susceptibilities recorded under zero-field-cooling condition have been fitted according to the Néel's expression for ferrimagnets. Subsequently, the molecular field constants and the corresponding exchange constants have been calculated. The fitting result shows that the magnetic interaction in the system becomes weaker as the annealing temperature rises. In addition, negative magnetization is observed during field-cooling process. The higher annealing temperature is beneficial to the growth of tetrahedral sublattice, leading to a decrease on compensation temperature. Furthermore, magnetization hysteresis loops for all the samples demonstrate the crucial role of grain size on the magnetic properties.     

Enhanced temperature stable dielectric properties and energy-storage density of BaSnO3-modified (Bi0.5Na0.5)0.94Ba0.06TiO3 lead-free ceramics

A series of (1-x)(Bi_0.5Na_0.5)_0.94Ba_0.06TiO₃-xBaSnO₃ (BNBT-100xBSN, x = 0–20) lead-free ceramics were synthesized using a conventional high-temperature solid-state reaction route. The effects of BaSnO₃ on the dielectric, ferroelectric and energy-storage performance of BNBT-BSN were systematically investigated. Temperature dependent permittivity curves indicated the obviously enhanced relaxor ferroelectric property. The introduction of BaSnO₃ reduced the temperature corresponding to the first dielectric anomaly, which facilitated the dielectric temperature stability. △ε'/ε'_150°C varied no more than 15% within the temperature range of up to 338 °C (45–383 °C) for BNBT-15BSN. A slimed P-E loop was obtained with the remnant polarization of 0.4 μC/cm² for BNBT-15BSN. Moreover, the breakdown field intensity of BNBT-BSN increased effectively from 80 kV/cm to 115 kV/cm. Therefore, an optimum energy-storage performance was obtained in BNBT-15BSN with the energy-storage density of 1.2 J/cm³ whose energy-storage efficiency reached 86.7%. Furthermore, the possible contributions of defect and vacancy to relaxation and conductance mechanism were discussed by studying the impedance and electric modulus. The results above indicated the BNBT-100xBSN be a promising lead-free candidate for energy-storage capacitors.     

The effects of Mg2+/Si4+ co-substitution for Al3+ on sintering and photoluminescence of (Gd,Lu)3Al5O12:Ce garnet ceramics

A series of phase-pure [(Gd_0.6Lu_0.4)_0.99Ce_0.01]₃[Al_1-z(Mg/Si)_z]₅O₁₂ (z = 0-0.10) garnet phosphor powders were prepared via gel-combustion, which were then sintered into ceramics (up to 1550 °C) under atmospheric pressure. Dilatometry revealed that equimole of Mg²⁺/Si⁴⁺ substitution for Al³⁺ accelerates densification and lowers the activation energy for grain boundary diffusion in the intermediate stage of sintering (∼1150–1370 °C), which was assayed to be ∼353 kJ/mol for z = 0 and ∼289 kJ/mol for z = 0.10. The acceleration effects of Mg²⁺/Si⁴⁺ on sintering and grain growth were further demonstrated by the results of ramp and holding sintering. Firing at 1550 °C for 4 h also produced ∼99 % dense ceramics for the Mg²⁺/Si⁴⁺ codoped garnet powders. Through considering crystal splitting of the Ce³⁺ 5d energy level, photon-phonon coupling, and crystal structure/microstructure, the influences of Mg²⁺/Si⁴⁺ content and material form on Ce³⁺ luminescence, including intensity, external/internal quantum efficiencies, emission wavelength, CIE color coordinates and decay time, were clarified in detail.     

Improved sintering behavior and microwave dielectric properties of SnO2-based ceramics and their LTCC materials with ultrawide temperature stability

Microwave dielectric ceramics with simple composition, a low permittivity (ε_r), high quality factor (Q × f) and temperature stability, specifically in the ultrawide temperature range, are vital for millimetre-wave communication. Hence, in this study, the improvements in sintering behavior and microwave dielectric properties of the SnO₂ ceramic with a porous microstructure were investigated. The relative density of the Sn_1-xTi_xO₂ ceramic (65.1%) was improved to 98.8%, and the optimal sintering temperature of Sn_1-xTi_xO₂ ceramics reduced from 1525 °C to 1325 °C when Sn⁴⁺ was substituted with Ti⁴⁺. Furthermore, the ε_r of Sn_1-xTi_xO₂ (0 ≤ x ≤ 1.0) ceramics increased gradually with the rise in x, which can be ascribed to the increase in ionic polarisability and rattling effects of (Sn_1-xTi_x)⁴⁺. The intrinsic dielectric loss was mainly controlled by r_c (Sn/Ti–O), and the negative τ_f of the SnO₂ ceramic was optimised to near zero (x = 0.1) by the Ti⁴⁺ substitution for Sn⁴⁺. This study also explored the ideal microwave dielectric properties (ε_r = 13.7, Q × f = 40,700 GHz at 9.9 GHz, and τ_f = ?7.2 ppm/°C) of the Sn_0.9Ti_0.1O₂ ceramic. Its optimal sintering temperature was decreased to 950 °C when the sintering aids (ZnO–B₂O₃ glass and LiF) were introduced. The Sn_0.9Ti_0.1O₂-5 wt% LiF ceramic also exhibited excellent microwave dielectric properties (ε_r = 12.8, Q × f = 23,000 GHz at 10.5 GHz, and τ_f = ?17.1 ppm/°C). At the ultrawide temperature range (?150 °C to +125 °C), the τ_ε of the Sn_0.9Ti_0.1O₂-5 wt% LiF ceramic was +13.3 ppm/°C, indicating excellent temperature stability. The good chemical compatibility of the Sn_0.9Ti_0.1O₂-5 wt% LiF ceramic and the Ag electrode demonstrates their potential application for millimetre-wave communication.     

Excellent temperature stability of strain in PZ-PT-BNT ternary ceramics

Lead-based Pb(Zr, Ti)O₃ ceramics have been widely applied in piezoelectric actuators, and yet high temperature stability and large strain have been pursued for further application. In this work, a novel PbZrO₃–PbTiO₃-(Bi_0.5Na_0.5)TiO₃ (PZ-PT-BNT) piezoelectric ceramic is designed and prepared by solid-state route. It is found that the introduction of BNT constituent enhances the relaxation behavior of PZ-PT ceramic, inhibits the abrupt change in dielectric properties near Curie temperature, and increases the proportion of tetragonal phase with high temperature stability. Meanwhile, the patterns of electric domains are intentionally modified by adjusting composition of PZ-PT-BNT. Short and broad electric domains in PZ-PT-0.03BNT ceramic are observed by piezoresponse force microscopy, which are insensitive to temperature and have faster response under electric field, contributing to strain characteristics. As a result, through integrating phase structure and electric domain configuration, a strain of 0.21% and excellent temperature stability where the variation of strain is less than 8% in the temperature range of 25–250 °C are achieved in PZ-PT-0.03BNT ceramic. The findings provide an effective strategy for improving the strain stability of PZ-PT-based piezoelectric ceramics, and demonstrate that PZ-PT-BNT ceramics have potential application prospects in high-temperature piezoelectric actuators.     

Pulse energy-storage performance and temperature stability of Bi2O3-added BaTiO3 based ceramics

The temperature stability and temperature stability range of barium titanate-based pulse energy-storage ceramics were modified by Bi₂O₃ tailoring in (Ba_0.98-xLi_0.02Bi_x) (Mg_0·04Ti_0.96)O₃ (x = 0, 0.025, 0.05, 0.075, 0.1) and (Ba_1.03-1.5xLi_0.02Bi_x) (Mg_0·04Ti_0.96)O₃ (x = 0.125, 0.15, 0.2, 0.25) ceramics. Excellent pulse energy-storage performances of ceramic films are achieved via the new dual priority strategy of establishing cationic vacancies and forming a liquid phase. The dielectric constant plateau appears due to the cubic phase and space charges. Outstanding temperature stability, frequency stability and antifatigue performance are obtained in the ceramics, and their variations are all less than 15%. The comprehensive energy-storage properties with dual priority parameters of energy-storage density and efficiency of 3.13 J/cm³ and 91.71%, accompanied by an excellent pulse discharge energy density of 2.48 J/cm³, current density of 1313.23 A/cm² and power density of 195.26 MW/cm³ are gained at x = 0.1. The perfect pulse energy-storage performances as well as ultrahigh stability are correlated with synergistic effects of multiphase coexistence, cubic phase, liquid-phase sintering, grain size, ceramic resistance, space charges and polar nanoregions. The comprehensive parameters indicate that the (Ba_0·88Li_0·02Bi_0.1) (Mg_0·04Ti_0.96)O₃ ceramics have potential application in high precision fields.     

Two low-permittivity melilite ceramics in the SrO-MO-GeO2 (M = Mg,Zn) system and their temperature stability through compositional modifications

Two melilite ceramics Sr₂AGe₂O₇ (A = Mg, Zn) with low permittivity were prepared by a solid-state reaction method. The crystal structure and microstructure of the ceramics were characterized by X-ray diffraction, transmission electron microscopy, Raman spectroscopy, and scanning electron microscopy. Both ceramics crystallized in a single melilite structure with a tetragonal space group P-42m (113) and exhibited homogeneous microstructures. Optimum microwave dielectric properties with relative permittivity (ε_r) of 8.56, quality factor (Q × f) of 28,800 GHz, and temperature coefficient of resonance frequency (τ_f) of −70.5 ppm/°C were obtained in Sr₂MgGe₂O₇ sintered at 1330 °C. Sr₂ZnGe₂O₇ possessed ε_r of 8.81, Q × f of 35,700 GHz, and τ_f of −84.4 ppm/°C when sintered at 1290 °C. Thermal stability of resonance frequency was accessible when the negative τ_f values of Sr₂AGe₂O₇ were adjusted after the formation of composite ceramics with CaTiO₃.     

Enhanced piezoelectricity and temperature stability in LaFeO3-modified KNN-based lead-free ceramics

(0.96-x)K_0.48Na_0.52NbO₃-0.04Bi_0.5Na_0.5ZrO₃-xLaFeO₃ ceramics (abbreviated as KNN-BNZ-LF1000x) with enhanced piezoelectric performance and temperature stability were prepared by the conventional solid-state sintering method. It was found that the incorporation of LaFeO₃ gradually shifted the O-T phase boundary toward room temperature, while maintaining the Curie temperature above 300°C. The optimal piezoelectricity was found at x = 0.006, with relatively high piezoelectric constant d₃₃ of 345 pC/N as well as a high level of unipolar strain (0.126% at 3 kV/mm). Benefiting from the diffused phase transition induced by appropriate amount of LaFeO₃ content, the KNN-BNZ-LF6 sample possessed greatly enhanced the temperature stability of , which varied less than 8% in the temperature range of 20°C-100°C.     

Achieving outstanding temperature stability in KNN-based lead-free ceramics for energy storage behavior

Lead-free ceramics with prominent energy storage properties are identified as the most potential materials accessed in the dielectric capacitors. Nevertheless, high recoverable energy storage density (W_rec), large energy storage efficiency (η) and preferable temperature stability can hardly be met simultaneously. The Bi(Zn_2/3Ta_1/3)O₃ and NaNbO₃ components are doped in KNN ceramics to substantiate the reliability of this tactic. A high recoverable energy density (W_rec) of ～ 4.55 J/cm³ and a large energy storage efficiency (η) of ～ 87.8% are acquired under the dielectric breakdown strength (DBS) of ～ 375 kV/cm, along with a splendid thermal stability (W_rec variation: ～ 2.3%, η variation: ～ 4.9%) within the temperature range of 20 ℃? 120 ℃. This article demonstrates that the KNN-based ceramics integrate high energy storage properties and outstanding temperature stability at the same time, which broadens the application fields of pulse power systems.     

The role of Al in the reactive synthesis of porous Mo2Ti2AlC3 ceramics

The mixed powders of TiH₂, molybdenum, aluminum and graphite with molar ratios of 2/2/n/2.85 (n ranges from 1.0 to 1.4 mol with an interval of 0.1 mol) were used as raw material powders for this work, and a novel porous Mo₂Ti₂AlC₃ was synthesized via reactive synthesis. Through systematic research on the pore structure parameters of porous Mo₂Ti₂AlC₃ prepared with different aluminum content, the results show that there is a clear correlation between the aluminum content and the pore structure parameters. With the aluminum content rising from 1.0 to 1.2 mol, the viscous permeability coefficient and pore size decreased, while the porosity increased; When the aluminum content increased from 1.2 to 1.4 mol, the pore structure parameters of porous Mo₂Ti₂AlC₃ displayed an opposite trend. The reasons for the evolution laws of these pore structure parameters were also discussed in depth. In addition, the pore structure forming mechanism of porous Mo₂Ti₂AlC₃ ceramics during the activation reaction sintering process has been explored. This work can provide an important reference for the subsequent preparation of quaternary porous MAX phase ceramics.