Low-temperature synthesis and microwave dielectric properties of trirutile-structure MgTa2O6 ceramics by aqueous sol–gel process

Trirutile-structure MgTa₂O₆ ceramics were prepared by aqueous sol–gel method and microwave dielectric properties were investigated. Highly reactive nanosized MgTa₂O₆ powders were successfully synthesized at 500 °C in oxygen atmosphere with particle sizes of 20–40 nm. The evolution of phase formation was detected by DTA–TG and XRD. Sintering characteristic and microwave dielectric properties of MgTa₂O₆ ceramics were studied at different temperatures ranging from 1100 to 1300 °C. With the increase of sintering temperature, density, ?_r and Q · f values increased and saturated at 1200 °C with excellent microwave properties of ?_r ～ 30.1, Q · f ～ 57,300 GHz and τ_f ～ 29 ppm/°C. The sintering temperature of MgTa₂O₆ ceramics was significantly reduced by aqueous sol–gel process compared to conventional solid-state method.     

Synthesis and microwave dielectric properties of pseudobrookite-type structure Mg5Nb4O15 ceramics by aqueous sol–gel technique

Pseudobrookite-type Mg₅Nb₄O₁₅ ceramics were prepared by aqueous sol–gel process and microwave dielectric properties were investigated. Highly reactive nanosized Mg₅Nb₄O₁₅ powders were successfully synthesized at 600 °C in oxygen atmosphere with particle sizes of 20–40 nm firstly and then phase evolution was detected by DTA-TG and XRD. Sintering characteristics and microwave dielectric properties of Mg₅Nb₄O₁₅ ceramics were studied at different temperatures ranging from 1200 °C to 1400 °C. With the increase of sintering temperature, density, ?_r and Q·f values increased, and then saturated at 1300 °C. Excellent microwave properties of ?_r ～11.3, Q·f ～43,300 GHz and τ_f ～?58 ppm/°C, were obtained finally. The sintering temperature of Mg₅Nb₄O₁₅ ceramics was significantly reduced by aqueous sol–gel process compared to conventional solid-state methods.     

Synthesis and microwave dielectric properties of CaSiO3 nanopowder by the sol–gel process

The synthesis and microwave dielectric properties of CaSiO₃ nanopowder by sol–gel method have been investigated in this paper. CaSiO₃ nanoparticles with an average grain size of 50–60 nm were obtained by calcining the CaO–SiO₂ xerogel that was prepared from Calcium nitrate tetrahydrate (Ca(NO₃)₂·4H₂O) and tetraethylortho silicate (TEOS). Calcining the CaO–SiO₂ xerogel at 1150 °C, the pseudowollastonite-CaSiO₃ phase was completely formed. However, the main phase is not CaSiO₃ or CaSi₂O₄ but SiO₂ when calcining the mixture of SiO₂ and CaCO₃ at 1150 °C. Comparing with CaO–SiO₂ ceramics prepared by solid-state process, the CaSiO₃ ceramics made from nanopowders calcined at 1000 °C achieved more compact structure at the sintering temperature of 1320 °C, and then had excellent microwave dielectric properties: ?_r = 6.69, Qf = 25398 GHz.     

Synthesis and electrochemical properties of LiV3O8 via an improved sol–gel process

LiV₃O₈ cathode material was synthesized via a hydrothermal improved sol–gel process using LiOH, NH₄VO₃ and oxalic acid as raw materials. The thermal decomposition process of the as-prepared LiV₃O₈ precursor was investigated by thermogravimetric (TG) and differential scanning calorimetry (DSC). The structure, morphology and electrochemical performance of the as-synthesized LiV₃O₈ samples were characterized by X-ray diffraction (XRD), Fourier transform infrared (FT-IR), scanning electron microscopy (SEM) and the galvanostatic charge–discharge test. The effects of synthesis conditions on phases, structure and electrochemical performance of the LiV₃O₈ samples were particularly discussed. Result shows that pure LiV₃O₈ sample can be obtained at 300 °C, which is much lower than that of normal citric assisted sol–gel method. The sample synthesized at 350 °C exhibits the best electrochemical performance, which can present an initial discharge capacity of 301.1 mAh/g at a current density of 50 mA/g and maintain 271.6 mA/g (about 90.2% of its initial value) after 10 cycles.     

Crystal structure and microwave dielectric properties of temperature stable (CoxZn1–x)TiNb2O8 ceramics

(Co_xZn_1–x)TiNb₂O₈ (x = 0.2–0.8) microwave dielectric ceramics were synthesized via the conventional solid-state reaction route, and the correlation of microwave dielectric properties on the crystal structure was discussed. Crystal structures of ceramic samples were systematically investigated by X-ray powder diffraction. Moreover, composition-induced phase transitions were confirmed via the following sequence: for x ≤ 0.2, single-phase orthorhombic ixiolite (ZnTiNb₂O₈) was formed, whereas for 0.3 ≤ x<0.8, ixiolite and rutile coexisted. When x ≥ 0.8, only single-phase rutile was detected. For the (Co_xZn_1–x)TiNb₂O₈ ceramics, the microwave dielectric properties were changed with the crystal structural transitions: the dielectric constant (ε_r) and the temperature coefficient of resonant frequency (τ_f) increased upon increasing the Co²⁺, but the quality factor (Q) decreased. A near-zero τ_f = +1.6 ppm/°C was obtained in the Co_0.38Zn_0.62TiNb₂O₈ ceramics with ε_r = 40.7 and high Q × f = 16 790 GHz. These research outcomes are expected to have great significance for developing microwave dielectric ceramics in practical applications.     

Structure and microwave dielectric properties of Ba1−xSrxMg2V2O8 ceramics

The Ba_1−xSr_xMg₂V₂O₈ (0≤x≤0.4) microwave dielectric ceramics were fabricated by a standard solid-state reaction method. The formation of a continuous solid solution within the whole composition range was identified. The ceramic samples could be well densified in the temperature range of 885–975 °C in air for 4 h. The permittivity ε_r was found to increase with increasing ionic polarizabilities. The Q×f values were believed to be closely related with packing fraction and grain refinement. The Sr²⁺ substitution contributed to a monotonous increase of the A-site bond valence, such that the τ_f value experienced a considerable variation from negative to positive values. The optimum microwave dielectric properties of an ε_r of 13.3, a high Qxf of 86,640 GHz (9.6 Hz) and a near-zero τ_f of −6 ppm/°C could be yielded in the x=0.15 sample when sintered at 915 °C for 4 h.     

Effects of Ni2+ substitution on the crystal structure,bond valence,and microwave dielectric properties of BaAl2–2xNi2xSi2O8–x ceramics

BaAl_2?2xNi_2xSi₂O_8?x (x = 0, 0.005, 0.01, 0.02, 0.03) ceramics were prepared using traditional solid phase reaction method. The microwave dielectric properties, including permittivity (ε_r), quality factor (Q × f), and temperature coefficient of resonant frequency (τ_f), were discussed based on the bond valence theory. The first-principle calculation was adopted to determine the site (Ba, Al, and Si) where doping element (Ni²⁺) would be inclined to occupy. The substitution of Ni²⁺ for Al³⁺ contributed to the breaking of Al-O and Si-O bonds and then facilitated the BaAl₂Si₂O₈ (BAS) hexacelsian-celsian transformation. Moreover, this substitution could change the bond strength between cation and oxygen anion due to the variation of the bond valence, which reasonably explained the variation of ε_r, Q × f, and τ_f values. Well-sintered and completely transformed celsian ceramics can be obtained after doping with Ni²⁺. When x = 0.01, compact BaAl_1.98Ni_0.02Si₂O_7.99 ceramic exhibited highly promising microwave dielectric properties: ε_r = 6.89, Q × f = 53, 287 GHz and τ_f = -25.31 × 10^?6 /°C.     

Crystal structure and microwave dielectric properties of Zn0.9Ti0.8−xSnxNb2.2O8 ceramics

The crystal structure and microwave dielectric properties of Zn_0.9Ti_0.8?xSn_xNb_2.2O₈ (x = 0.00, 0.05, 0.10, 0.15) ceramics sintered at temperatures ranging from 1100 °C to 1140 °C for 6 h were investigated. A single phase with ixiolite structure was obtained. With the increase of Sn content, the dielectric constant decreased attributed to the decrease of dielectric polarizability. The Qf value decreased with the decrease of packing fraction and grain size. The temperature coefficient of resonant frequency (τ_f) increased due to the increase of the bond valence of Zn_0.9Ti_0.8?xSn_xNb_2.2O₈ ceramics. The excellent microwave dielectric properties of ? = 35.05, Qf = 49,100 GHz, τ_f = ?27.6 × 10^?6/°C were obtained for Zn_0.9Ti_0.8?xSn_xNb_2.2O₈ (x = 0.05) specimens sintered at 1120 °C for 6 h.     

Phase composition,crystal structure and microwave dielectric properties of Mg2−xCuxSiO4 ceramics

In this work, the Mg_2-xCu_xSiO₄(x = 0–0.40) microwave dielectric ceramics were prepared using solid-state reaction method. Compared with the Mg₂SiO₄ sample, the Cu-substituted Mg samples could be sintered at a lower temperature. The Mg_2?xCu_xSiO₄ ceramics exhibit the composite phases of Mg₂SiO₄ and a small quantity of MgSiO₃. The Cu²⁺ ion presented a solid solution with the Mg₂SiO₄ phase and preferentially occupy Mg(1) site. The distortion of MgO₆ octahedron was modified by Cu²⁺ ions, resulting in a positive change in the temperature coefficient of resonance frequency (τ_f) values. Excellent microwave dielectric properties of ε_r = 6.35, high Qf of ～ 188,500 GHz and near zero τ_f = ?2.0 ppm/°C were achieved at x = 0.08 under sintering at 1250 °C for 4 h. Thus, the fabricated ceramics were considered as possible candidates for millimeter-wave device applications.     

Preparation,structure and microwave dielectric properties of novel La2MgGeO6 ceramics with hexagonal structure and adjustment of its τf value

A novel La₂MgGeO₆ ceramic was synthesized through a solid-state reaction process within a sintering temperature range of 1450–1550 °C. By a combination of X-ray diffraction and Rietveld refinement analyses, the ceramics were found to have a pure hexagonal phase structure belonging to space group R3/146. The scanning electron microscopy images revealed that the ceramic grains were closely connected. The effects of internal (lattice energy, valence bond, and fraction packing) and external factors (density) on the microwave properties of ceramics were also studied. The ceramic exhibited excellent microwave dielectric performances, with a relative permittivity (?_r) of 21.2, a quality factor (Q × f) of 52 360 GHz, and a temperature coefficient of resonant frequency (τ_f) of ?44.2 ppm/°C, when sintered at 1500 °C for 4 h. The τ_f value of the La₂MgGeO₆ ceramic doped with CaTiO₃ could be adjusted to zero. Particularly, 0.2La₂MgGeO₆-0.8CaTiO₃ ceramics have good microwave dielectric properties with τ_f = +2.1 ppm/°C, Q × f = 15 610 GHz, and ?_r = 40.3.     

Synthesis and modification of silica-based epoxy nanocomposites with different sol–gel process enhanced thermal and mechanical properties

This research article describes the results of nano-silica composites filled with different epoxy contents containing nano-SiO₂ particles from (5–25 wt%). Reinforcing hybrid composites enhance thermal and mechanical properties to achieve vital and sustainable products. Silica-based nanocomposites with high purity were prepared and used for the surface modification of nanosized silica particles. The surface structure's composition and physical properties of modified nano-SiO₂ particles were characterized through Fourier transferred infrared spectrometer, X-ray photoelectron spectroscopy, thermogravimetric analyzer, and scanning electron microscopic. Silica-based nanocomposites were prepared by incorporating of modified nano-SiO₂ as an enhancing filler. The morphology of fracture surface and dynamic mechanical properties were investigated. Results showed that the silica-based epoxy nanocomposites are bearing a long chain structure that could improve the compatibility of silica nanocomposites with epoxy resin and contribute to a better dispersion state in the matrix, which enhanced the overall performance of epoxy-cured products.     

Structure and microwave dielectric properties of BaAl2−2xLi2xSi2O8-2x ceramics

BaAl_2-2xLi_2xSi₂O_8-2x (x = 0, 0.005, 0.0075, 0.01, 0.02, 0.03) ceramics were synthesized by solid-state sintering method. Based on density functional theory, the first-principle calculations provided by the Cambridge Sequential Total Energy Package (CASTEP) software were introduced to the BaAl₂Si₂O₈ (BAS) system. In an effort to confirm the site occupied by Li⁺, we discussed the formation energy and final energy of different positions of Li⁺ doped BAS. The result demonstrated that Li⁺ should substitute Al³⁺ to promote the hexacelsian-to-celsian transformation with the aid of generated oxygen vacancies. The sintering behavior, crystal structure, surface appearance, and microwave dielectric properties of samples were investigated. Completely transformed celsian could be obtained when x = 0.005–0.03, which lowered the sintering temperature from 1400 °C (x = 0) to 1300 °C (x = 0.03), as well as strikingly improved the compactness, quality factor (Q × f) value and temperature coefficient of resonant frequency (τ_f) of BAS ceramics. When x = 0.1, unveiling the significant effects of Al-position ion substitution, BaAl_1.98Li_0.02Si₂O_7.98 ceramic sintered at 1350 °C for 5 h exhibited a supreme Q × f value of 48,620 GHz, and the ε_r and τ_f values were 6.99 and -23.29 × 10^?6 °C^?1, respectively.     

Structure characterization and microwave dielectric properties of LiGa5O8 ceramic with low-εr and low loss

LiGa₅O₈ ceramics with inverse spinel structure were prepared in a temperature range of 1200–1300 ℃ by solid-state reaction method. LiGa₅O₈ ceramics crystallized in cubic structure with space group P4₃32, in which Li⁺ and Ga³⁺ distributed in the octahedral B sites with 1:3 ordering. The optimal microwave dielectric properties with ε_r =10.51, Q × f = 127,040 GHz, and τ_f = –60.16 ppm/℃ were achieved at 1260 ℃ for 6 h. Microwave dielectric properties were discussed in combination with the intrinsic characteristics of crystal structure by packing fraction, Raman spectra, and infrared reflectivity spectrum. Additionally, CaTiO₃ was used to suppress τ_f of LiGa₅O₈ ceramics to near zero, and optimized performances of ε_r = 12.79, Q × f = 109,752 GHz and τ_f = +4.07 ppm/℃ were obtained for 0.94LiGa₅O₈‐0.06CaTiO₃ ceramics at 1260 ℃. These bright spots make LiGa₅O₈ ceramic a potential candidate for 5 G and millimeter wave technology.     

Sintering behaviour and microwave dielectric properties of BaAl2−2x(ZnSi)xSi2O8 ceramics

BaAl_2?2x(ZnSi)_xSi₂O₈ (x = 0.2–1.0) ceramics were prepared using the conventional solid-state reaction method. The sintering behaviour, phase composition and microwave dielectric properties of the prepared compositions were then investigated. All compositions showed a single phase except for x = 0.8. By substituting (Zn_0.5Si_0.5)³⁺ for Al³⁺ ions, the optimal sintering temperatures of the compositions decreased from 1475 °C (x = 0) to 1000 °C (x = 0.8), which then slightly increased to 1100 °C (x = 1.0). Moreover, the phase stability of BaAl₂Si₂O₈ was improved. A novel BaZnSi₃O₈ microwave dielectric ceramic was obtained at the sintering temperature of 1100 °C. This ceramic possesses good microwave dielectric properties with ε_r = 6.60, Q × f = 52401 GHz (at 15.4 GHz) and τ_f = ?24.5 ppm/°C.     

Crystal structure of corundum type Mg4(Nb2–xTax)O9 microwave dielectric ceramics with low dielectric loss

New microwave dielectric ceramics, i.e. Mg₄(Nb_2−xTa_x)O₉ (MNT) solid solutions, were synthesized and their microwave dielectric properties and crystal structure were investigated in this study. From the discrete variational Xα (DV-Xα) method, it was found that the Ta–O bonds in the TaO₆ octahedron become more covalent than Nb–O bonds in the NbO₆ octahedron; this result leads to the decrease of the ionicity in the Ta⁵⁺ ion. The dielectric constants of MNT were slightly decreased from 12.4 to 11.5; this result might be due to the covalent interaction of Ta–O bonding. The quality factors of the samples were found to exhibit high value (Q·f≒350 000 GHz for x=2) which is comparable to those of Al₂O₃.     

Synthesis of Lu2Ti2O7 nano-powders by salt modified sol–gel process

Nano-sized Lu₂Ti₂O₇ powders have been prepared successfully by a chloride salt modified sol–gel process, by using tetrabutyl titanate and lutecium nitrate as precursors. The results indicate that salt precipitated during the synthesis process can form a thin layer of salt crust on the surface of the newly formed nano-particles and prevent re-agglomeration and hinder the particle growth resulting in well-dispersed Lu₂Ti₂O₇ nano-crystals. However, the increased salt contents can also lead to the significant size increase of the formed particles. Meanwhile, different types of salt species differently affect on the particle morphologies. Based on the above observation, well-dispersed spherical Lu₂Ti₂O₇ nano-crystals with an average particle size of about 50 nm can be obtained at 850 °C by the modified sol–gel process with precursor to NaCl ratio of 1:15.     

Phase structure,band gap and microwave dielectric properties of Ba8Ti3Nb4−xSbxO24 ceramics

High dielectric constant and low loss ceramics in the Ba₈Ti₃Nb_4?xSb_xO₂₄ (x=0–2) system were prepared by conventional solid-state ceramic route. As x increased from 0 to 1.5, a single phase with hexagonal 8H perovskite structure was formed and the band gap values increased from 3.38 to 3.47 eV. However, the Sb₂O₃ secondary phase was detected as the x reached 2. The optimum sintering temperature was reduced from 1460 to 1380 °C, the quality factors (Q×f) were effectively enhanced from 22,900 to 38,000 GHz and τ_f was significantly lowered from 110 ppm/°C to 2 ppm/°C, whereas the dielectric constant decreased from 49 to 35. A good combined microwave dielectric properties with ε_r=37.5, Q×f=38,000 GHz, τ_f=15 ppm/°C were obtained for x=1.5.     

Crystal structure,phase compositions,and microwave dielectric properties of malayaite-type Ca1−xSrxSnSiO5 ceramics

Low-permittivity Ca_1−xSr_xSnSiO₅ (0 ≤ x ≤ 0.45) microwave dielectric ceramics were prepared via traditional state-reaction at 1400°C-1450°C for 5 hours. Moreover the microwave dielectric properties of SnO₂ ceramic were obtained for the first time. SnO₂ ceramic was difficult to densify, and SnO₂ ceramic (ρ_rel = 65.1%) that was sintered at 1525°C exhibited the optimal microwave dielectric properties of ε_r = 5.27, Q × f = 89 300 GHz (at 14.5 GHz), and τ_f = −26.7 ppm/°C. For Ca_1−xSr_xSnSiO₅ (0 ≤ x ≤ 0.15) ceramics, Sr²⁺ could be dissolved in the Ca²⁺ site of Ca_1−xSr_xSnSiO₅ to form a single phase, and the partial substitution of Ca²⁺ by Sr²⁺ could improve the microwave dielectric properties of CaSnSiO₅ ceramic. Secondary phases (SnO₂ and SrSiO₃) appeared at 0.2 ≤ x ≤ 0.45 and could adjust the abnormally positive τ_f value of CaSnSiO₅ ceramic. The highest Q × f value (60 100 GHz at 10.4 GHz) and optimal microwave dielectric properties (ε_r = 9.42, Q × f = 47 500 GHz at 12.4 GHz, and τ_f = −1.2 ppm/°C) of Ca_1−xSr_xSnSiO₅ ceramics were obtained at x = 0.05 and 0.45, respectively.     

Influence of Li2O–B2O3–SiO2 glass on the sintering behavior and microwave dielectric properties of BaO–0.15ZnO–4TiO2 ceramics

This paper reports the investigation of the performance of Li₂O–B₂O₃–SiO₂ (LBS) glass as a sintering aid to lower the sintering temperature of BaO–0.15ZnO–4TiO₂ (BZT) ceramics, as well as the detailed study on the sintering behavior, phase evolution, microstructure and microwave dielectric properties of the resulting BZT ceramics. The addition of LBS glass significantly lowers the sintering temperature of the BZT ceramics from 1150 °C to 875–925 °C. Small amount of LBS glass promotes the densification of BZT ceramic and improves the dielectric properties. However, excessive LBS addition leads to the precipitation of glass phase and growth of abnormal grain, deteriorating the dielectric properties of the BZT ceramic. The BZT ceramic with 5 wt% LBS addition sintered at 900 °C shows excellent microwave dielectric properties: ε_r=27.88, Q×f=14,795 GHz.