Mechanical and dielectric properties of reduced graphene oxide nanosheets/alumina composite ceramics

Reduced graphene oxide (rGO) nanosheets/alumina (Al₂O₃) composite ceramics were fabricated by hot-pressing sintering. The density, porosity, microhardness, flexural strength and complex permittivity were investigated to study their mechanical and dielectric properties. The results revealed that the rGO nanosheets were uniformly distributed in the Al₂O₃ matrix and that the composite ceramics were highly dense at 3.67–3.99 g/cm³. Due to low rGO hardness and elevated porosity, the microhardness exhibits a decreasing trend as the rGO content increases. The flexural strength first increased and then decreased with the escalation of rGO content, and the highest strength of 313.75 MPa was obtained at 3 wt%, increasing by 37.61% relative to that of the hot-pressing sintered Al₂O₃ ceramic. Owing to the enhanced interfacial polarization, dipole polarization, polarization relaxation loss and conductance loss, the real part and imaginary part of complex permittivity increase from 10.40 to 52.73 and from 0.08 to 28.86 as the rGO content rose from 0 wt% to 4 wt%, respectively.     

Dielectric properties of manganese and cobalt doped lead iron tantalate ceramics

This paper reports the results of synthesis and sintering studies as well as dielectric properties of Pb(Fe_1/2Ta_1/2)O₃ (PFT) relaxor ferroelectric ceramics. Influence of doping with MnO₂ and Co₃O₄ (0.1–1 mol%) on resistivity and dielectric characteristics were investigated. The dielectric permittivity and dissipation factor of the ceramics were determined as a function of temperature in the range from −55 to 500 °C at frequencies 10 Hz to 1 MHz. DC resistivities of the samples were measured in the temperature range 20–500 °C. Two maxima in dielectric permittivity versus temperature curves were observed, dependent on frequency and the content of dopants. The investigated PFT ceramics were characterized by high dielectric permittivity of 3500–6700 at the transition temperature and 900–17,000 at the second maxima.     

Design and fabrication of Al2O3f/SiCN composite with excellent microwave absorbing and mechanical properties

A new kind of structural and functional integration ceramic matrix composite material was prepared from high-performance alumina (Al₂O₃) fibers and absorbing silicon carbonitride (SiCN) ceramics via a combination of polymer infiltration pyrolysis (PIP) and chemical vapor infiltration (CVI) methods. The Al₂O₃ fiber annealed at its cracked temperature had enhanced permittivity, because the sizing agent on the Al₂O₃ fiber surface was cracked into pyrolysis carbon. For PIP + CVI Al₂O_3f/SiCN composites, PIP SiCN matrix with low conductivity was used as the matching phase, while CVI SiCN matrix with medium permittivity and dielectric loss was regarded as the reinforcing phase distributed in porous PIP SiCN matrix and inter-bundles of Al₂O₃ fiber to improve their mechanical and microwave absorption properties. The fracture toughness and flexural strength of Al₂O_3f/SiCN composite were determined to be 9.4 ± 0.5 MPa m^1/2 and 279 ± 28 MPa, respectively. Based on the design principles for impedance matching, the Al₂O_3f/SiCN composites before and after oxidation were used as loss and impedance layers, respectively. It was found that the optimized composite had the lowest reflection coefficient (RC) of −70 dB and the effective absorption bandwidth covering the whole X-band. In conclusion, Al₂O_3f/SiCN composite can serve as a high-temperature structural material with excellent microwave absorption properties for aerospace applications.     

0.73ZrTi2O6–0.27MgNb2O6 microwave dielectric ceramics modified by Al2O3 addition

0.73ZrTi₂O₆–0.27MgNb₂O₆ ceramics with various Al₂O₃ contents (0‐2.0 wt%) were prepared by conventional ceramic route. The effects of Al₂O₃ on the phase composition, microstructure, conductivity, and microwave dielectric properties were systematically investigated. The coexistence of a disordered α–PbO₂‐type phase and a rutile second phase was found in all compact ceramics with low Al₂O₃ contents (x = 0, 0.5, and 1.0 wt%), while a corundum phase was detected when Al₂O₃ additive increased to 1.5 and 2.0 wt% based on X‐ray diffraction results. With the addition of Al₂O₃, the decreased grain size of the matrix phase was observed using field‐emission scanning electron microscope, accompanied with increased resistivity and band‐gap energy. Additionally, Al₂O₃ additives efficiently improved the quality factor of the ceramics. After sintering at 1360°C for 3 hours, the ceramic with 1.0 wt% Al₂O₃ exhibited excellent microwave dielectric properties: a dielectric constant of 43.8, a quality factor of 33 900 GHz (at 6.6 GHz), and a near‐zero temperature coefficient of resonant frequency (3.1 ppm/^°C).     

Significantly improved dielectric properties of TiO2 ceramics through acceptor-doping and Ar/H2 annealing

The acceptor-doped rutile TiO₂ ceramics, x mol% M₂O₃-(1-x) mol% TiO₂ (M = Al³⁺, Ga³⁺, and In³⁺), were prepared by solid state reaction method. The influence of Ar/H₂ annealing on the structural and dielectric properties of the ceramics were systematically investigated. Our results reveal that the dielectric properties of the ceramics can be significantly improved by the Ar/H₂ annealing. Ga³⁺ is found to be the most suitable dopant with the best doping level of 5 mol%. Excellent dielectric properties of colossal and flat dielectric permittivity (~1.2 × 10⁵ (@1 kHz and 25 °C), low dielectric loss (~0.1), and good frequency stability were achieved over the temperature range of -70–150 °C in the Ar/H₂-annealed 5 mol% Ga₂O₃-95 mol% TiO₂ ceramic. This approach of acceptor-doping and Ar/H₂ annealing leads to two thermally activated relaxations in the sample. The low-temperature relaxation is argued to be a Maxwell-Wagner relaxation caused by frozen electrons, while the high-temperature relaxation is a glass-transition-like relaxation associated with the freezing process of the electrons. This work highlights that engineering low-temperature Maxwell-Wagner relaxation paves a new way other than the frequently used acceptor-donor dual doping to design superior dielectric properties in the TiO₂ system.     

Dielectric Properties of Ultra‐Low Sintering Temperature Al2O3–BBSZ Glass Composite

Ceramic composites of B₂O₃–Bi₂O₃–SiO₂–ZnO (BBSZ) glass mixed with Al₂O₃ (10–50 vol%) were sintered at 450°C, and their microstructural and dielectric properties investigated. Dense structures were obtained when the Al₂O₃ content was lower than 30 vol%. Raman, XRD, and FESEM showed the existence of a secondary phase, Bi₂₄Si₂O₄₀, in all samples. The dielectric properties of the composite with 30 vol% addition of Al₂O₃ showed good dielectric properties with ε_r of 14.8 and 20.8 and 32.5 at 100 kHz and 100 MHz and 1 GHz, respectively. The tanδ values at the same frequencies were 0.004 and 0.006 and 0.016. The results show that BBSZ glass with different amounts of Al₂O₃ exhibit widely applicable relative permittivity values and affordable loss and are thus promising candidates for ultra‐low sintering temperature applications.     

Enhanced dielectric characteristics of Ba0.94Bi0.04(Fe0.5Nb0.5)O3 coated with SiO2 and SiO2/Al2O3 over a broad frequency and temperature range

Pure phase of Ba_0.94Bi_0.04(Fe_0.5Nb_0.5)O₃ (BBFN) nano-particles were obtained by chemical co-precipitation method. The core-shell structure of BBFN@SiO₂ and BBFN@SiO₂/Al₂O₃ particles and the target ceramics were successfully prepared by aqueous chemical coating approach. The microstructures and dielectric properties of BBFN@SiO₂ and BBFN@SiO₂/Al₂O₃ were studied. Both the BBFN@SiO₂ and BBFN@SiO₂/Al₂O₃ samples show significantly decreased dielectric loss and good frequency and temperature stability on relative permittivity. Compared to the rapid decline of relative permittivity of BBFN@SiO₂, the synergistic effect of SiO₂ and Al₂O₃ in BBFN@SiO₂/Al₂O₃ ceramics made the relative permittivity of which remains a relatively high level with very low dielectric loss, making it more suitable in colossal permittivity applications. Based on the impedance analysis, the grain boundary effect and IBLC models play the important role for the improvement of dielectric properties of BBFN@SiO₂/Al₂O₃ samples.     

Structural and dielectric properties,and nonlinear electrical response of the CaCu3-xZnxTi4O12 ceramics: Experimental and computational studies

CaCu_3-xZn_xTi₄O₁₂ ceramics (x = 0, 0.05, 0.10) were successfully prepared by a conventional solid-state reaction method. Their structural and dielectric properties, and nonlinear electrical response were systematically inspected. The X-ray diffraction results indicated that single-phase CaCu₃Ti₄O₁₂ (JCPDS no. 75–2188) was obtained in all sintered ceramics. Changes in the lattice parameter are well-matched with the computational result, indicating an occupation of Zn²⁺ doping ions at Cu²⁺ sites. The overall tendency shows that the average grain size decreases when x increases. Due to a decrease in overall grain size, the dielectric permittivity of CaCu_3-xZn_xTi₄O₁₂ decreases expressively. Despite a decrease in the dielectric permittivity, it remains at a high level in the doped ceramics (~3,406–11,441). Besides retention in high dielectric permittivity, the dielectric loss tangent of x = 0.05 and 0.10 (~0.074–0.076) is lower than that of x = 0 (~0.227). A reduction in the dielectric loss tangent in the CaCu_3-xZn_xTi₄O₁₂ ceramics is closely associated with the enhanced grain boundary response. Increases in grain boundary resistance, breakdown electric field, and conduction activation energy of grain boundary as a result of Zn²⁺ substitution are shown to play a crucial role in improved grain boundary response. Furthermore, the XPS analysis shows the existence of Cu⁺/Cu²⁺ and Ti³⁺/Ti⁴⁺, indicating charge compensation due to the loss of oxygen lattice. Based on all results of this work, enhanced dielectric properties of the Zn-doped CCTO can be explained using the internal barrier layer capacitor model.     

Growth of Al2O3–PTFE composite film at room temperature by aerosol deposition method

To fabricate a ceramic-based substrate for 3-dimensional integration modules with a thick film coating process at room temperature, aerosol deposition method was employed. Al₂O₃ was chosen as a main coating material for the requirements of low permittivity and dielectric loss. Especially to give a functionality of plasticity, composite film with polytetrafluoroethylene (PTFE) was also studied. The effects of PTFE, which was incorporated in the film, were investigated by the microstructural characterization. It was confirmed that Al₂O₃–PTFE film with the grain size of 100–200 nm were grown at room temperature using Al₂O₃–0.5 wt% PTFE mixture powders. Dielectric constant and dielectric loss of Al₂O₃–PTFE film were 4.5 and 0.005 at 1 MHz, respectively.     

Microwave processing and properties of ceramics with different dielectric loss

Microwave sintering behaviors of three kinds of ceramics with different dielectric loss [Al₂O₃, Ce–Y–ZrO₂ and lead-based relaxor ferroelectrics (PMZNT)] in 2·45 GHz microwave furnace were described. Measurement of sample densities showed an enhancement of the sintering processing for all materials studied. For PMZNT and Ce–Y–ZrO₂ with high dipolar loss or ionic conductive loss, the associated microstructure examined using scanning electron microscopy showed that microwave-sintered compacts produced much finer grain sizes at near theoretical density compared to conventional sintering. Resulting material properties, such as flexure strength and breakdown strength, were also increased due to developed microstructure in microwave processing. However, a comparable grain size and properties were observed for high pure Al₂O₃ with low dielectric loss in microwave and conventional methods. ©     

On the fabrication and mechanical properties of Si3N4 ceramics with low content sintering additives

Si₃N₄ ceramics were prepared by hot pressing (HP) and spark plasma sintering (SPS) methods using low content (5 mol%) Al₂O₃–RE₂O₃(RE = Y, Yb, and La)–SiO₂/TiN as sintering additives/secondary additives. The effects of sintering additives and sintering methods on the composition, microstructures, and mechanical properties (hardness and fracture toughness) were investigated. The results show that fully density Si₃N₄ ceramics could be fabricated by rational tailoring of sintering additives and sintering method, and TiN secondary additive could promote the density during HP and SPS. Besides, SN-AYS-SPS possesses the most competitive mechanical properties among all the as-prepared ceramics with the Vickers hardness as 17.31 ± .43 GPa and fracture toughness as 11.07 ± .48 MPa m^1/2.     

Dielectric and microwave absorption properties of FeSiAl/Al2O3 composites containing FeSiAl particles of different sizes

Here in, the effects of FeSiAl particle size on the dielectric and microwave absorption properties of FeSiAl/Al₂O₃ composites were studied. FeSiAl/Al₂O₃ composites containing 18–25 μm, 25–48 μm, and 48–75 μm FeSiAl particles were prepared by hot-pressed sintering based on uniformly mixed FeSiAl and Al₂O₃ powders. Results show that the real permittivity and the imaginary permittivity are significantly promoted with increasing FeSiAl particle size, which is ascribed to the enhanced interfacial polarization and conductance loss. In addition, the favorable matching impedance and suitable attenuation coefficient enabled the composite containing 25–48 μm FeSiAl powder to show a minimum reflection loss of ?34.4 dB at 11.7 GHz and an effective absorption bandwidth (<-10 dB) of 1.4 GHz in 11.0–12.4 GHz, when the thickness is 1.1 mm. By adjusting the thickness to 1.4 mm, the effective absorption bandwidth of the composite reaches a maximum value of 2.0 GHz in the 8.3–10.3 GHz range, indicating tunable, strong, and highly efficient microwave absorption performance.     

Good dielectric performance and broadband dielectric polarization in Ag,Nb co-doped TiO2

Due to the demand of miniaturization and integration for ceramic capacitors in electronic components market, TiO₂-based ceramics with colossal permittivity has become a research hotspot in recent years. In this work, we report that Ag⁺/Nb⁵⁺ co-doped (Ag_1/4Nb_3/4)_xTi_1−xO₂ (ANTOx) ceramics with colossal permittivity over a wide frequency and temperature range were successfully prepared by a traditional solid–state method. Notably, compositions of ANTO0.005 and ANTO0.01 respectively exhibit both low dielectric loss (0.040 and 0.050 at 1 kHz), high dielectric permittivity (9.2 × 10³ and 1.6 × 10⁴ at 1 kHz), and good thermal stability, which satisfy the requirements for the temperature range of application of X9R and X8R ceramic capacitors, respectively. The origin of the dielectric behavior was attributed to five dielectric relaxation phenomena, i.e., localized carriers' hopping, electron–pinned defect–dipoles, interfacial polarization, and oxygen vacancies ionization and diffusion, as suggested by dielectric temperature spectra and valence state analysis via XPS; wherein, electron-pinned defect–dipoles and internal barrier layer capacitance are believed to be the main causes for the giant dielectric permittivity in ANTOx ceramics.     

Colossal dielectric permittivity in (Al+Nb) co-doped Ba0.4Sr0.6TiO3 ceramics

Stimulated by the outstanding colossal permittivity behavior achieved in trivalent and pentavalent cations co-doped rutile TiO₂ ceramics, the co-doping effects on the dielectric behavior of Ba_0.4Sr_0.6TiO₃ ceramics were further explored. In this work, (Al + Nb) co-doped Ba_0.4Sr_0.6TiO₃ ceramics were synthesized via a standard solid state ceramic route. The structural evolution was analyzed using X-ray diffraction patterns and Raman spectra. Dense microstructures with no apparent change of grain morphology were observed from the scanning electron microscopy. A huge enhancement of dielectric permittivity was obtained with 1 mol% (Al + Nb) doping and excellent dielectric performances (ε_r ∼ 20,000, tanδ ∼ 0.06 at 1 kHz) were achieved after further heat treatment. The formation of electron pinned defect dipoles localized in grains may account for the optimization of dielectric behaviors and the corresponding chemical valence states were confirmed from the XPS results.     

TiN/Al2O3 composites and graded laminates thereof consolidated by spark plasma sintering

A rapid consolidation process named Spark Plasma Sintering (SPS) has been applied to compact duplex TiN/Al₂O₃ composites and graded laminates thereof. Fully or nearly fully compacted samples were prepared at 1500 °C with a holding time of 3 min under a pressure of 75 MPa. The unusually high grain-growth rate of Al₂O₃ occurring in monolithic Al₂O₃ at this sintering temperature is prevented by the addition of TiN particles. Crack-free graded laminates with distinct interfaces between layers were prepared by loading samples inside the die, both symmetrically and asymmetrically. The observed mechanical properties, e.g. hardness and fracture toughness, are related to the microstructural features of the compacted samples.     

Effect of substituting Al3+ for Ti4+on the microwave dielectric performance of Mg2Ti1-xAl4/3xO4 (0.01 ≤ x ≤ 0.09) ceramics

In this paper, Mg₂Ti_1-xAl_4/3xO₄ ceramics (0.01 ≤ x ≤ 0.09) were synthesized through conventional solid-state ceramic route. The cubic spinel structure, microstructure and microwave properties of Mg₂Ti_1-xAl_4/3xO₄ (x = 0.01, 0.03, 0.05, 0.07, 0.09) ceramics were investigated by X-ray diffraction, Raman spectra, infrared spectra. Rietveld refinements confirm that a spinel structure phase with space group Fd-3m is formed. The variation of the permittivity was concerned with the ionic polarizability, and the value of τ_f was influenced by the bond valence. Both Q × f values and relative density showed an identical trend. Intrinsic properties of Mg₂Ti_1-xAl_4/3xO₄ ceramics were analyzed by infrared spectra and Raman spectra. In addition, the Mg₂Ti_1-xAl_4/3xO₄ ceramic sintered at 1420 °C for 4 h possessed optimal dielectric properties (ε_r = 14.65, Q × f = 182347 GHz, τ_f = −57.7 ppm/°C) when x = 0.09.     

Preparation of Al2O3 coating on TiN coating by polymer-assisted deposition to improve oxidation resistance in coking inhibition applications

In order to inhibit the metal catalytic coking and improve oxidation resistance of single TiN coating, the TiN/Al₂O₃ double layer coatings were designed as a chemically inert coating for methylcyclohexane supercritical pyrolysis. Internal TiN coatings were prepared by atmospheric pressure chemical vapor deposition using TiCl₄–H₂–N₂ system. The external Al₂O₃ coatings with different thicknesses were prepared on the TiN surface by polymer-assisted deposition, and the coating with the most suitable thickness was further annealed at different temperatures of 600, 700, 800 and 900 °C. The morphology, elemental and phase composition of TiN/Al₂O₃ coatings were characterized by SEM, EDX and XRD respectively. The chemical state information of the coating elements was based on Ti 2p, Al 2p core level X-ray photoelectron spectroscopy (XPS) spectra. The results indicated that the external Al₂O₃ coating will partially peel off at 900 °C annealing temperature. The thermogravimetric analysis results indicated that all TiN/Al₂O₃ coatings show better oxidation resistance than single-layer TiN coating. The anti-coking test with methylcyclohexane supercritical pyrolysis showed that the TiN/Al₂O₃ coatings can effectively cover the metal catalytic sites and eliminate metal catalytic coking. However, the acid sites of external Al₂O₃ coating slightly promoted coking, so the anti-coking ratios of TiN/Al₂O₃ coatings were smaller than that of TiN. Thus, the addition of external Al₂O₃ coating can greatly improve the oxidation resistance of TiN coatings with little loss of coking resistance.     

Optimization of microstructure and mechanical properties of oscillatory pressure sintered ZrO2–Al2O3-SiCp ceramics

Zirconia ceramic is a significant structural material, but its use under some extreme circumstances is limited by its mechanical properties. In this work, SiC particles (SiCp) were added into alumina toughened zirconia ceramics to prepare ZrO₂–Al₂O₃-SiCp ceramics with high performance by using oscillatory pressure sintering (OPS). Results showed that the best OPS temperature of 1600 °C was obtained, and the optimal SiCp particle size and content were 200 nm and 10 vol% respectively. Under these conditions, the specimen exhibited higher mechanical properties including Vickers hardness of 15.43 GPa, bending strength of 1162 MPa and fracture toughness of 6.36 MPa m^1/2. Moreover, it was found that the atomic matching between ZrO₂/SiCp, Al₂O₃/SiCp, and ZrO₂/Al₂O₃ was much higher, showing the coherent interface relationship. Therefore, it was favorable for enhanced mechanical properties of as-prepared ZrO₂–Al₂O₃-SiCp ceramics.     

Structure Evolution and Enhanced Microwave Dielectric Characteristics of (Sr1−xCax)La2Al2O7 Ceramics

(Sr_1?xCa_x)La₂Al₂O₇ (0.1 ≤ x ≤ 0.5) ceramics were prepared by a standard solid‐state reaction method. Their densification behavior and microwave dielectric properties were investigated together with the structural evolution. X‐ray diffraction analysis indicated that the major phase of Ruddlesden–Popper structure with n = 2 was obtained for all the compositions investigated here. Partial Ca substitution improved the sintering behavior of SrLa₂Al₂O₇ ceramics. More importantly, microwave dielectric characteristics were enhanced in (Sr_1?xCa_x)La₂Al₂O₇ ceramics with compositions of x = 0.1~0.3. The stacking fault was confirmed by TEM observation in the present ceramics, and the microwave dielectric loss was influenced by it. The best combination of microwave dielectric characteristics was achieved for the composition of x = 0.1: ε_r = 19.9, Qf = 135 400 GHz and τ_f = ?18.5 ppm/°C.