MnO2对Ba(Mg1/3Nb2/3)O3微观结构和微波介电性能的影响

研究了MnO2助烧剂对Ba(Mg1/3Nb2/3)O3陶瓷的微观结构和微波介电性能.MnO2可以有效地使Ba(Mg1/3Nb2/3)O3陶瓷的致密化温度由1550℃降低到1400℃左右.随MnO2掺量的增加,Ba(Mg1/3Nb2/3)O3陶瓷的12超晶格衍射峰的强度减弱,但是没有第二相出现.1400℃烧结4h陶瓷的晶粒尺寸在1.5μm左右.MnO2的掺入改善了Ba(Mg1/3Nb2/3)O3陶瓷的微波介电性能,MnO2掺量为1%mol的Ba(Mg1/3Nb2/3)O3陶瓷具有最好的微波介电性能εr≈31.5,Qf=68000,τf=3.11×10-5/℃,这可归功于陶瓷具有相当高的相对密度.     

预烧温度对BZN微波陶瓷介电性能的影响

以工业纯BaCO3、ZnO、Nb2O5为原料,按照一定配比配料混合,通过传统的固相反应法合成Ba(Zn1/3Nb2/3)O3(即BZN)陶瓷材料,预烧温度(分别为1000、1100和1200℃)对BZN陶瓷微波性能的影响过程中,对合成的BZN粉体进行差热/热重分析,对烧结后的BZN陶瓷进行XRD分析和SEM形貌观察,利用矢量网络分析仪测量BZN陶瓷的微波性能Q、εr和rf.实验结果表明,预烧温度对BZN微波陶瓷的介电性能影响比较大,预烧温度为1200℃时可以获得较好的介电性能εr=41.6,Q*f=38671GHz,τf=2.8×105/℃.     

Phase developments in the Pb(Zn1/2W1/2)O3-Pb(Zn1/3Ta2/3)O3-Pb(Zn1/3Nb2/3)O3 pseudo-ternary system

The phase stability ranges in the B-site precursor (Zn_1/2W_1/2)O₂-(Zn_1/3Ta_2/3)O₂-(Zn_1/3Nb_2/3)O₂ were determined by X-ray diffraction (XRD), where wolframite, tri-αPbO₂, and columbite phases were identified. Next attempts were carried out (with the addition of PbO) for the system Pb(Zn_1/2W_1/2)O₃-Pb(Zn_1/3Ta_2/3)O₃-Pb(Zn_1/3Nb_2/3)O₃, where the perovskite phase did not develop in the entire compositions investigated. Instead, only the Pb₂WO₅ and pyrochlore phases (along with ZnO) resulted.     

Raman spectroscopy and cathodoluminescence characteristics of order-disorder Ba(Zn1/3Ta2/3)O3 ceramics

The order-disorder transition in Ba(Zn_1/3Ta_2/3)O₃ (BZT) was characterized by using Raman spectroscopy, transmission electron microscopy (TEM), and cathodoluminescence (CL) microscopy. The 1:2 ordered structure of pure BZT ceramics was replaced by a 1:1 ordered structure at 1650 °C and the 1:1 ordered structure of BZT sintered at 1650 °C exhibited a 1:2 ordered structure when it was reannealed at 1500 °C for 12 h. The A_1g lines in the Raman spectrum of the sintered and reannealed samples were shifted to lower and higher wavenumbers, respectively. From the CL analysis, the 1:1 ordered BZT exhibited mainly three emission bands at around 533.2 (2.32 eV), 599.1 (2.07 eV), and 682.1 nm (1.81 eV), whereas the 1:2 ordered BZT exhibited mainly five bands at 346.4 (3.58 eV), 427.5 (2.90 eV), 520.9 (2.38 eV), 593.0 (2.09 eV), and 678.9 nm (1.82 eV). The strongest band originating from 2.32 to 2.38 eV was broadened, and the band center shifted towards a higher and lower wavelength in the 1:1 and 1:2 ordered BZT, respectively. Additional bands at around 346 and 427 nm in the grain interior of the annealed sample were strongly related to the 1:2 ordering of BZT.     

Piezoelectric shear-mode properties of Pb(Yb1/2Nb1/2)O3-PbTiO3 ceramics

A Pb(Yb_1/2Nb_1/2)O₃-PbTiO₃ [PYNT] solid solution was synthesized and characterized for its potential use. The shear-mode dielectric and piezoelectric behaviors of PYNT with a morphotropic phase boundary (MPB) composition were studied as a function of temperature. Dielectric permittivity K₁₁^T and loss were found to be 2310 and 2.5%, respectively, at room temperature. Piezoelectric coefficient d₁₅ and electromechanical coupling factor k₁₅ were calculated to be 710 pC/N and 0.70, respectively, maintaining nearly constant up to 300 °C, resistivity and RC time constant were observed to be 2.4 × 10⁹ Ω cm and 1.07 s, respectively, at 350 °C. These good piezoelectric properties, together with the high Curie temperature (T_c ∼ 370 °C), indicate that PYNT is a promising candidate for high temperature-shear sensor and inkjet actuator applications.     

Effect of Pb(Fe1/2Nb1/2)O3 modification on dielectric and piezoelectric properties of Pb(Mg1/3Nb2/3)O3-PbZr0.52Ti0.48O3 ceramics

10 mol% Pb(Fe_1/2Nb_1/2)O₃ (PFN) modified Pb(Mg_1/3Nb_2/3)O₃-PbZr_0.52Ti_0.48O₃ (PMN-PZT) relaxor ferroelectric ceramics with compositions of (0.9 − x)PMN-0.1PFN-xPZT (x = 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8 and 0.9) were prepared. X-ray diffraction investigations indicated that as-prepared ceramics were of pure perovskite phase and the sample with composition of x = 0.8 was close to morphotropic phase boundary (MPB) between rhombohedral and tetragonal phase. Dielectric properties of the as-prepared ceramics were measured, and the Curie temperature (T_c) increased sharply with increasing PZT content and could be higher than 300 °C around morphotropic phase boundary (MPB) area. At 1 kHz, the sample with composition of x = 0.1 had the largest room temperature dielectric constant ?_r = 3519 and maximum dielectric constant ?_m = 20,475 at T_m, while the sample with composition of x = 0.3 possessed the maximum dielectric relaxor factor of γ = 1.94. The largest d₃₃ = 318 pC/N could be obtained from as-prepared ceramics at x = 0.9. The maximum remnant polarization (P_r = 28.3 μC/cm²) was obtained from as-prepared ceramics at x = 0.4.     

Effect of CuO addition to Nd(Zn1/2Ti1/2)O3 ceramics on sintering behavior and microwave dielectric properties

The microwave dielectric properties and microstructures of CuO-doped Nd(Zn_1/2Ti_1/2)O₃ ceramics prepared by the conventional solid-state route were investigated. The prepared Nd(Zn_1/2Ti_1/2)O₃ exhibits a mixture of Zn and Ti showing 1:1 order in the B-site. As an appropriate sintering aid, not only did CuO lower the sintering temperature, it could effectively hold back the evaporation of Zn in the Nd(Zn_1/2Ti_1/2)O₃. Moreover, CuO only resided in boundaries, which was confirmed by EDX analysis. The measured lattice parameters of CuO-doped Nd(Zn_1/2Ti_1/2)O₃ (a = 5.4652 ± 0.0005 ?, b = 5.6399 ± 0.0007 ?, c = 7.7797 ± 0.0008 ? and β = 90.01 ± 0.01°) retained identical to that of the pure Nd(Zn_1/2Ti_1/2)O₃ in all cases. In comparison with the pure Nd(Zn_1/2Ti_1/2)O₃ ceramics, specimen with 1 wt.% CuO addition possesses a compatible combination of dielectric properties with a ε_r of 30.68, a Q × f of 158,000 GHz (at 8 GHz) and a τ_f of − 45 ppm/°C at 1270 °C. It also indicated a 60 °C lowering in the sintering temperature. The proposed dielectrics can be a very promising candidate material for microwave or millimeter wave applications requiring extremely low dielectric loss.     

Ag and O ion irradiation induced improvement in dielectric properties of the Ba(Co1/3Nb2/3)O3 thin films

We present the preliminary results of temperature and frequency dependent dielectric measurements on Ba(Co_1/3Nb_2/3)O₃ (BCN) thin films. These films were prepared on indium tin oxide (ITO) coated glass substrates by the pulse laser deposition (PLD) technique. It exhibits single-phase hexagonal symmetry. These films were irradiated with Ag¹⁵⁺ (200 MeV) and O⁷⁺ (100 MeV) beams at the fluence 1 × 10¹¹, 1 × 10¹², and 1 × 10¹³ ions/cm². On irradiating these films, its dielectric constant (?′) and dielectric loss (tan δ) parameters improve compared to un-irradiated film. Compared to O⁷⁺ irradiation induced point/cluster defects Ag¹⁵⁺ induced columnar defects are more effective in reducing/pinning trapped charges within grains. The present paper highlights the role of swift heavy ion irradiation in engineering the dielectric properties of conductive samples to enable them to be useful for microwave device applications.     

Microwave dielectric characteristics of Ba(Mg1/3Ta2/3)O3 ceramics sintered at low-temperatures

The microwave dielectric properties and microstructures of Ba(Mg_1/3Ta_2/3)O₃ (BMT) ceramics sintered at low temperatures with 2–3 wt.% NaF additives were investigated. BMT ceramics sintered at 1340 °C for 3–12 h showed dielectric constants (_r) of 25.5–25.7, Qf values of 41 500–50 400 GHz and temperature coefficients of the resonator frequency (τ_f) of 10.9–21.4 ppm °C⁻¹. The variation of sintering time almost had no effect on the dielectric constant. The Qf value increased and the τ_f decreased with increasing sintering time. The ordering degree of Mg²⁺ and Ta⁵⁺ at B-sites increased with increasing sintering time.     

Structure and ferroelectric properties of Bi(Zn1/2Ti1/2)O3-(Bi1/2K1/2)TiO3 perovskite solid solutions

Lead-free piezoelectric ceramics based on χBi(Zn_1/2Ti_1/2)O₃-(1-χ)(Bi_1/2K_1/2)TiO₃ were obtained via solid state processing techniques. A single perovskite phase with tetragonal symmetry was obtained for Bi(Zn_1/2Ti_1/2)O₃ (BZT) substitutions up to 20 mol%. The maximum density was 97.1% at the composition of χ = 0.1. The dielectric measurement indicated that the transition temperature decreased linearly with increasing BZT content. The P-E loops revealed an increase in remanent polarization (P_r) with the addition of BZT. The maximum planar coupling coefficient, κ_r, for the χ = 0.1 composition was 21.6 and the piezoelectric coefficient, d₃₃, for χ = 0, χ = 0.05, and χ = 0.1 was 108, 185, and 235 pm/V, respectively. Overall, the dielectric and piezoelectric properties showed significant improvement when BZT was added.     

Ba(Zn1/3Nb2/3)O3/Ni0.8Zn0.2Fe2O4 magneto-dielectric composite with large dielectric constant and high permeability

Ba(Zn_1/3Nb_2/3)O₃/Ni_0.8Zn_0.2Fe₂O₄ (BZN/NZO) composites were synthesized via the conventional solid-state reaction method. The phase composition and surface morphology of the composites were investigated using XRD and SEM, respectively. The dielectric and magnetic properties of the composites were studied. The results show that the BZN/NZO composites have large dielectric constants and very high permeabilities. For the 20%BZN/80%NZO composite, the dielectric constant and permeability in low frequency range are about 8,000 and 18, respectively. The large dielectric behavior of the BZN/NZO composites is mainly attributed to the Maxwell–Wagner polarization.     

Effects of Mn doping on the structure and electrical properties of high-temperature BiScO3-PbTiO3-Pb(Zn1/3Nb2/3)O3 piezoelectric ceramics

The effects of Mn addition on the structure, ferroelectric, and piezoelectric properties of the 0.35BiScO₃-0.60PbTiO₃-0.05Pb(Zn_1/3Nb_2/3)O₃ ceramics were studied. The results demonstrate that the addition of small amounts of Mn did not cause a remarkable change in crystal structure, but resulted in an evident evolution in microstructure and ferro-piezoelctric properties. The addition of Mn can induce combinatory “hard” and “soft” piezoelectric characteristics due to aliovalent substitutions. The optimal electrical properties are obtained in the 0.25 mol% Mn-doped composition with a high Curie temperature, indicating that Mn doping contributes to the electrical properties of the ceramics. It can be expected that the improved piezoelectric material can be a promising candidate for high-temperature piezoelectric applications.     

Synthesis and properties of Ba(Zn1/3Ta2/3)O3 for microwave and millimeter wave applications

High dielectric materials have gained an important position in microwave electronics by reducing the size and cost of components for a wide range of applications from mobile telephony to spatial communications. Ba(Zn_1/3Ta_2/3)O₃ (BZT) is an A(B′B″)O₃ type perovskite material, showing ultra high values of the quality factor Q. Ceramic-based BZT dielectric materials were prepared by solid state reaction. The samples were sintered at temperatures in the range 1400 ÷ 1600 °C for 4 h. Compositional, structural and morphological characterization were performed by using XRD, SEM and EDX analysis. The dielectric properties were measured in the microwave range (6 ÷ 7 GHz). An additional annealing at 1400 °C for 10 h has improved some dielectric parameters. For samples sintered at temperatures higher than 1500 °C, the permittivity values were obtained in the interval 30 ÷ 35 and almost do not change the value after the annealing. The Q × f product substantially increases up to about 135,000 GHz, exhibiting a low temperature coefficient of the resonant frequency (τ_f) in microwaves. The best parameters were obtained for the samples sintered at 1600 °C with additional annealing. The achieved high values of the Q × f product recommend these materials for microwave and millimeter wave applications.     

Crystallographic and dielectric properties of barium-substituted Pb(Mg1/3Ta2/3)O3 ceramics

Ceramic powders of (Ba,Pb)Pb(Mg_1/3Ta_2/3)O₃ were prepared via a B-site precursor route. Crystal symmetries and lattice parameters were determined. Monophasic perovskite was developed after the two-step reaction process, in which the lattice parameters showed linear changes in the entire composition range. Dielectric responses of the ceramics with compositional and frequency changes were investigated. The results were also compared with the (Ba,Pb)(Zn_1/3Ta_2/3)O₃ data.     

Electrical properties of Pb(Mg1/3Nb2/3)O3-PbTiO3 ceramics modified with WO3

Ferroelectrics 0.67Pb (Mg_1/3Nb_2/3)O₃-0.33PbTiO₃ (PMN-PT) + x mol% WO₃ (x=0.1, 0.5, 1, 2) were prepared by columbite precursor method. Electrical properties of WO₃-modified ferroelectrics were investigated. X-ray diffraction (XRD) was used to identify crystal structure, and pyrochlore phase were observed in 0.67Pb (Mg_1/3Nb_2/3)O₃-0.33PbTiO₃+2 mol% WO₃. Dielectric peak temperature decreased with WO₃ doping, indicating that W⁶⁺ incorporated into PMN-PT lattice. Lattice constant, pyrochlore phase and grain size contribute to the variation of K_max. Both piezoelectric constant (d₃₃) and electromechanical coupling factors (k_p) were enhanced by doping 0.1 mol% WO₃, which results from the introduction of “soft” characteristics into PMN-PT, while further WO₃ addition was detrimental. We consider that the two factors, introduction of “soft” characteristics and the formation of pyrochlore phase, appear to act together to cause the variation of piezoelectric properties of 0.67PMN-0.33PT ceramics doping with WO₃.     

Crystallographic and dielectric properties of the Pb2(MgW)O6-La1.33(MgW)O6 solid solutions

A continuous series of solid solutions was found to form with a perovskite structure in the given system. At room temperature the unit cells were cubic in the 1–65 mol% La_1.33(MgW)O₆ region and pseudotetragonally distorted in the 75–100 mol% La_1.33(MgW)O₆ region. In the latter region, an ordering of A-site vacancies was found to occur along alternate c-planes. The Curie temperature decreased rapidly with increasing La_1.33(MgW)O₆ content up to 10 mol%.     

Microstructure effect on the properties of electrostrictive Pb(Mg1/3Nb2/3)O3-PbTiO3 ceramics

We have studied the effect of the mechanical activation of the starting oxide mixture on the particle size of the resulting powders and the microstructure of electrostrictive lead magnesium niobate-lead titanate ceramics. The results demonstrate that reducing the grain size of the ceramics reduces their dielectric permittivity in both weak and strong electric fields, reduces their electrostrictive coefficient M ₁₁, shifts the processes related to polarization saturation to higher electric fields, and increases the dielectric and electromechanical hystereses.     

Dielectric properties of Ba0.6Sr0.4TiO3-Sr(Ga0.5Ta0.5)O3 solid solutions

Ba_0.6Sr_0.4TiO₃-Sr(Ga_0.5Ta,sub>0.5)O₃ solid solutions are prepared by a solid-state reaction method, and their dielectric and tunable characteristics are investigated. The solid solutions with cubic perovskite structures are obtained for compositions of 10-50 mol% Sr(Ga_0.5Ta_0.5)O₃. It is observed that the addition of Sr(Ga_0.5Ta_0.5)O₃ into Ba_0.6Sr,sub>0.4TiO₃ causes a shift in the phase transition peak to a lower temperature. Ba_0.6Sr_0.4TiO₃-Sr(Ga_0.5Ta,sub>0.5)O₃ solid solutions exhibit depressed and broadened phase transition peaks, resulting in decreased dielectric constants and dielectric losses at room temperature. With the increase of Sr(Ga_0.5Ta_0.5)O₃ content, the dielectric constant, loss tangent, and tunability are decreased. 0.9Ba_0.6Sr_0.4TiO₃-0.1Sr(Ga_0.5Ta,sub>0.5)O₃ has a dielectric constant ϵ = 534 and a tunability of 16% at 100 kHz under 2.63 kV/mm. The dielectric characteristics of Ba_0.6Sr_0.4TiO₃-Sr(Ga_0.5Ta,sub>0.5)O₃ ceramics at microwave frequencies are also evaluated.     

Mn-doping effect on dielectric and electromechanical losses in the system Pb(ZrxTi1?x)O3–Pb(Zn1/3Nb2/3)O3

Absract Dielectric and electromechanical losses play a critical role in the performance of the transducer in high power conditions. In this study, we report a systematic study on the effect of Mn-doping on the losses in the Pb(Zr _x Ti_1−x )O₃–Pb(Zn_1/3Nb_2/3)O₃ (PZT–PZN) system. Two types of sintering conditions were employed to synthesize ceramics with varying grain sizes. The Zr/Ti ratio in the PZT system was fixed at 52/48 corresponding to morphotropic phase boundary (MPB) and Mn concentration was varied from 0 to 0.9 wt%. The results show that the composition 0.9PZT–0.1PZN + 0.5 wt% Mn provides optimized magnitude for the dielectric, piezoelectric, and loss properties.     

Depolarization temperature and piezoelectric properties of Na1/2Bi1/2TiO3-Na1/2Bi1/2(Zn1/3Nb2/3)O3 ceramics by two-stage calcination method

A new group of NBT-based lead-free piezoelectric ceramics, Na_1/2Bi_1/2TiO₃-Na_1/2Bi_1/2(Zn_1/3Nb_2/3)O₃, was synthesized using the two-stage calcination method and depolarization temperatures and piezoelectric properties were also investigated. The XRD analysis showed that the ceramics system had a morphotropic phase boundary (MPB) between the rhombohedral and the tetragonal structure. The highest piezoelectric properties of d ₃₃ = 97 pC/N and k _t = 0·46 were obtained near MPB compositions. Furthermore, the depolarization temperatures near MPB compositions were slightly decreased and the lowest T _d was maintained at 210°C.