Piezoelectric and dielectric properties of Dy2O3-doped (Bi0.5Na0.5)0.94Ba0.06TiO3 lead-free ceramics

(Bi_0.5Na_0.5)_0.94Ba_0.06TiO₃ + x wt% Dy₂O₃ with x = 0-0.3 ceramics were synthesized by conventional solid-state processes. The effects of Dy₂O₃ on the microstructure, the piezoelectric and dielectric properties were investigated. X-ray diffraction pattern confirmed that the coexistence of tetragonal and rhombohedral phases in the (Bi_0.5Na_0.5)_0.94Ba_0.06TiO₃ composition was not changed by adding 0.05-0.3 wt% Dy₂O₃. SEM images indicate that all the ceramics have pore-free microstructures with high density, and that doping of Dy₂O₃ inhibits the grain growth of the ceramics. The addition of Dy₂O₃ shows the double effects on decreasing the piezoelectric and dielectric properties for 0 < x < 0.15 when Dy³⁺ ions substitute B-site Ti⁴⁺ ions, and increasing the properties for 0.15 < x < 0.3 when Dy³⁺ ions enters into A-site of the perovskite structure. The optimum electric properties of piezoelectric constant d₃₃ = 170 pC/N and the dielectric constant ?_r = 1900 (at a frequency of 1 kHz) are obtained at x = 0.3.     

Polymorphic phase transition-induced electrical behavior of BiCoO3-modified (K0.48Na0.52)NbO3 lead-free piezoelectric ceramics

(1 − x)(K_0.48Na_0.52)NbO₃-xBiCoO₃ [KNN-xBC] lead-free piezoelectric ceramics were prepared by the conventional solid-state sintering method. The effects of the BiCoO₃ addition on the phase structure, dielectric, piezoelectric and ferroelectric properties of KNN-xBC ceramics were systematically investigated. The polymorphic phase transition (PPT) from rhombohedral to orthorhombic phase around room temperature was identified in the composition range of 0.01 ≤ x ≤ 0.02, and the improved electrical properties were induced by this PPT. The KNN-0.01BC ceramics near PPT exhibit optimum electrical properties: d₃₃ ∼ 165 pC/N, k_p ∼ 0.40, P_r ∼ 31.0 μC/cm², and E_c ∼ 12.6 kV/cm. These results indicate that the enhanced piezoelectric properties for alkali niobate can be achieved by forming the coexistence of rhombohedral and orthorhombic phases.     

Microstructure, ferroelectric, and piezoelectric properties of (1 − x − y)Bi0.5Na0.5TiO3-xBaTiO3-yBi0.5Ag0.5TiO3 lead-free ceramics

Lead-free (1 − x − y)Bi_0.5Na_0.5TiO₃-xBaTiO₃-yBi_0.5Ag_0.5TiO₃ (BNT-BT-BAT-x/y, x = 0-0.10, y = 0-0.075) piezoelectric ceramics were synthesized by conventional oxide-mixed method. The microstructure, ferroelectric, and piezoelectric properties of the ceramics were investigated. Results show that a morphotropic phase boundary (MPB) between rhombohedral and tetragonal phases of BNT-BT-BAT-x/0.04 ceramics is formed at x = 0.06-0.08. The addition of BAT has no obvious change on the crystal structure of BNT-BT ceramics while it causes the grain size of the ceramics to become more homogenous. Near the MPB, the ceramics with x = 0.06 and y = 0.05-0.06 possess optimum electrical properties: P_r ∼ 42.5 μC/cm², E_c ∼ 32.0 kV/cm, d₃₃ ∼ 172 pC/N, k_p ∼ 32.6%, and k_t ∼ 52.6%. The temperature dependences of k_p and polarization versus electric hysteresis loops reveal that the depolarization temperature (T_d) of BNT-BT-BAT-0.06/y ceramics decreases with increasing y. In addition, the polar and non-polar phases may coexist in the BNT-BT-BAT-x/y ceramics above T_d.     

The studies of phase relation, microstructure, magnetic transition, magnetocaloric effect in (Gd1−xErx)5Si1.7Ge2.3 compounds

The phase relation, microstructure, Curie temperatures (T_C), magnetic transition, and magnetocaloric effect of (Gd_1−xEr_x)₅Si_1.7Ge_2.3 (x = 0, 0.05, 0.1, 0.15, and 0.2) compounds prepared by arc-melting and then annealing at 1523 K (3 h) using purity Gd (99.9 wt.%) are investigated. The results of XRD patterns and SEM show that the main phases in those samples are mono-clinic Gd₅Si₂Ge₂ type structure. With increase of Er content from x = 0 to 0.2, the values of magnetic transition temperatures (T_C) decrease linearly from 228.7 K to 135.3 K. But the (Gd_1−xEr_x)₅Si_1.7Ge_2.3 compounds display large magnetic entropy near their transition temperatures in a magnetic field of 0-2 T. The maximum magnetic entropy change in (Gd_1−xEr_x)₅Si_1.7Ge_2.3 compounds are 24.56, 14.56, 16.84, 14.20, and 13.22 J/kg K⁻¹ with x = 0, 0.05, 0.1, 0.15, and 0.2, respectively.     

Characterization of sol-gel synthesised lead-free (1 − x)Na0.5Bi0.5TiO3-xBaTiO3-based ceramics

The crystal structure, microstructure, dielectric and ferroelectric properties of (1 − x)Na_0.5Bi_0.5TiO₃-xBaTiO₃ ceramics with x = 0, 0.03, 0.05, 0.07 and 0.1 are investigated. A structural variation according to the system composition was investigated by X-ray diffraction (XRD) analyses. The results revealed that the synthesis temperature for pure perovskite phase powder prepared by the present sol-gel process is much lower (800 °C), and a rhombohedral-tetragonal morphotropic phase boundary (MPB) is found for x = 0.07 composition which showing the highest remanent polarization value and the smallest coercive field. The optimum dielectric and piezoelectric properties were found with the 0.93Na_0.5Bi_0.5TiO₃-0.07BaTiO₃ composition. The piezoelectric constant d₃₃ is 120 pC/N and good polarization behaviour was observed with remanent polarization (P_r) of 12.18 pC/cm², coercive field (E_c) of 2.11 kV/mm, and enhanced dielectric properties ?_r > 1500 at room temperature. The 0.93Na_0.5Bi_0.5TiO₃-0.07BaTiO₃-based ceramic is a promising lead-free piezoelectric candidate for applications in different devices.     

Low temperature sintering and microwave dielectric properties of (Mg0.7Zn0.3)0.95Co0.05TiO3 ceramics with BaCu(B2O5) additions

The effects of BaCu(B₂O₅) additives on the sintering temperature and microwave dielectric properties of (Mg_0.7Zn_0.3)_0.95Co_0.05TiO₃ ceramics were investigated. The (Mg_0.7Zn_0.3)_0.95Co_0.05TiO₃ ceramics were not able to be sintered below 1000 °C. However, when BaCu(B₂O₅) were added, they were sintered below 1000 °C and had the good microwave dielectric properties. It was suggested that a liquid phase with the composition of BaCu(B₂O₅) was formed during the sintering and assisted the densification of the (Mg_0.7Zn_0.3)_0.95Co_0.05TiO₃ ceramics at low temperature. BaCu(B₂O₅) powders were produced and used to reduce the sintering temperature of the (Mg_0.7Zn_0.3)_0.95Co_0.05TiO₃ ceramics. Good microwave dielectric properties of Q × f = 35,000 GHz, ?_r = 18.5.0 and τ_f = −51 ppm/°C were obtained for the (Mg_0.7Zn_0.3)_0.95Co_0.05TiO₃ ceramics containing 7 wt.% mol% BaCu(B₂O₅) sintered at 950 °C for 4 h.     

Relationships between Zr substitution for Ti and microwave dielectric properties in Mg(ZrxTi1−x)O3 ceramics

The influence of Zr substitution for Ti on the microwave dielectric properties and microstructures of the Mg(Zr_xTi_1−x)O₃(MZ_xT) (0.01 ≤ x ≤ 0.3) ceramics was investigated. The quality factors of Mg(Zr_xTi_1−x)O₃ ceramics with x = 0.01-0.05 were improved because the solid solution of a small amount of Zr⁴⁺ substitution in the B-site could increase density and grain size. An excess of Zr⁴⁺ resulted in the formation of a great deal of secondary phase that declined the microwave dielectric properties of MZ_xT ceramics. The temperature coefficient of resonant frequency (τ_f) of Mg(Zr_xTi_1−x)O₃ ceramics slightly increased with increasing Zr content, and the variation in τ_f was attributed to the formation of secondary phases.     

Dielectric relaxation behaviors of pure and Pr6O11-doped CaCu3Ti4O12 ceramics in high temperature range

Pure and Pr₆O₁₁-doped CaCu₃Ti₄O₁₂ (CCTO) ceramics were prepared by conventional solid-state reaction method. The compositions and structures were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM). The influences of Pr-ion concentration on dielectric properties of CCTO were measured in the ranges of 60 Hz-3 MHz and 290-490 K. The third phase of Ca₂CuO₃ was observed from the XRD of CCTO ceramics. From SEM, the grain size was decreased obviously with high valence Pr-ion (mixing valence of Pr³⁺ and Pr⁴⁺) substituting Ca²⁺. The room temperature dielectric constant of Pr-doped CCTO ceramics, sintered at 1323 K, was an order of magnitude lower than the pure CCTO ceramics due to the grain size decreasing and Schottky potential increasing. The dielectric spectra of Pr-doped CCTO were flatter than that of pure CCTO. The loss tangent of Pr-doped CCTO ceramics was less than 0.20 in 2 × 10²-10⁵ Hz region below 440 K. The complex impedance spectra of pure and Pr-doped CCTOs were fitted by ZView. From low to high frequency, three semicircles were observed corresponding to three different conducting regions: electrode interface, grain boundary and grain. By fitting the resistors R and capacitors C, the activation energies of grain boundary and electrode contact were calculated. All doped CCTOs showed higher activation energies of grain boundary and electrode than those of pure CCTO ceramics, which were concordant with the decreasing of dielectric constant after Pr₆O₁₁ doping.     

Enhancement microwave dielectric properties of La(Mg0.5Sn0.5)O3 ceramics by substituting Mg with Ni

The microwave dielectric properties of La(Mg_0.5−xNi_xSn_0.5)O₃ ceramics were examined with a view to their exploitation for mobile communication. The La(Mg_0.5−xNi_xSn_0.5)O₃ ceramics were prepared by the conventional solid-state method at various sintering temperatures. The X-ray diffraction patterns of the La(Mg_0.4Ni_0.1Sn_0.5)O₃ ceramics revealed no significant variation of phase with sintering temperatures. Apparent density of 6.71 g/cm³, dielectric constant (?_r) of 20.19, quality factor (Q × f) of 74,600 GHz, and temperature coefficient of resonant frequency (τ_f) of −85 ppm/°C were obtained for La(Mg_0.4Ni_0.1Sn_0.5)O₃ ceramics that were sintered at 1550 °C for 4 h.     

Resistivity, thermopower, and thermal conductivity of nickel doped compounds Cr1−xNixSb2 at low temperatures

Substitutional compounds Cr_1−xNi_xSb₂ (0 ≤ x ≤ 0.1) were synthesized, and the effect of Ni substitution on transport and thermoelectric properties of Cr_1−xNi_xSb₂ were investigated at the temperatures from 7 to 310 K. The results indicated that the magnitudes of the resistivity and thermopower of Cr_1−xNi_xSb₂ decreased greatly with increasing Ni content at low temperatures, owing to an increase in electron concentration caused by Ni substitution for Cr. Experiments also showed that the low-temperature lattice thermal conductivity of Cr_1−xNi_xSb₂ decreased substantially with increasing Ni content due to an enhancement of phonon scattering by the increased number of Ni atoms. As a result, the figure of merit, ZT, of lightly doped Cr_0.99Ni_0.01Sb₂ was improved at T > ∼230 K. Specifically, the ZT of Cr_0.99Ni_0.01Sb₂ at 310 K was approximately ∼29% larger than that of CrSb₂, indicating that thermoelectric properties of CrSb₂ can be improved by an appropriate substitution of Ni for Cr.     

Effect of dwell time during sintering on piezoelectric properties of (Ba0.85Ca0.15)(Ti0.90Zr0.10)O3 lead-free ceramics

In this letter, the effect of dwell time (1-6 h) during sintering on the piezoelectric properties is investigated for the (Ba_0.85Ca_0.15)(Ti_0.90Zr_0.10)O₃ ceramics. All ceramics sintered at different dwell time are of a pure phase, and its structure distortion is induced by too long dwell time. Their dielectric constant and remanent polarization increases and the coercive field decreases with increasing dwell time. An enhanced piezoelectric behavior (d₃₃ ∼ 492 pC/N and k_p ∼ 51.5%) is demonstrated for the BCTZ ceramic with an optimum dwell time of 5 h, owing to the structure distortion together with a dense microstructure and a larger grain size.     

Preparation and luminescent characteristics of Sr3RE2(BO3)4:Dy (RE = Y, La, Gd) phosphors for white LED

Dysprosium-activated Sr₃RE₂(BO₃)₄ (RE = Y, La, Gd) phosphors were synthesized by a high temperature solid-state reaction method. The phase uniformity of the phosphors was characterized by X-ray powder diffraction (XRD) and the luminescence characteristics were investigated. The excitation spectra at 575 nm emission show strong spectral bands in the region of 300-500 nm. The emission spectra of the phosphors with 365 nm excitation show three bands centered at 484 nm, 575 nm and 680 nm, which originate from the transitions of ⁴F_9/2 → ⁶H_15/2, ⁴F_9/2 → ⁶H_13/2 and ⁴F_9/2 → ⁶H_11/2 of Dy³⁺, respectively. The effect of Dy³⁺ concentration on the emission intensity of the phosphors was investigated. The fluorescence decay curves for ⁴F_9/2 → ⁶H_13/2 excited at 365 nm and monitored at λ_em of 575 nm were measured. The decay times decreased slowly with increasing Dy³⁺ doping concentration due to a trap capturing to resonance fluorescence transfer of the activated ions and due to the exchange interactions between activated ion pairs. In order to determine the type of interaction between activated ions, the concentration dependence curves (lg(I/x) versus lg x) of Sr₃RE₂(BO₃)₄:Dy³⁺ (RE = Y, La, Gd) were plotted. The concentration quenching mechanism of the ⁴F_9/2 → ⁶H_13/2 (575 nm) transition of Dy³⁺ is the d-d interaction. All results indicate these phosphors are promising white-color luminescent materials.     

Effect of addition of Ba(W0.5Cu0.5)O3 in Pb(Mg1/3Nb2/3)O3-Pb(Zn1/3Nb2/3)O3-Pb(Zr0.52Ti0.48)O3 ceramics on the sintering temperature, electrical properties and phase transition

In this work, we report on the Pb(Mg_1/3Nb_2/3)O₃-Pb(Zn_1/3Nb_2/3)O₃-Pb(Zr_0.52Ti_0.48)O₃ (PMN-PZN-PZT) ceramics with Ba(W_0.5Cu_0.5)O₃ as the sintering aid that was manufactured in order to develop the low-temperature sintering materials for piezoelectric device applications. The phase transition, microstructure, dielectric, piezoelectric properties, and the temperature stability of the ceramics were investigated. The results showed that the addition of Ba(W_0.5Cu_0.5)O₃ significantly improved the sintering temperature of PMN-PZN-PZT ceramics and could lower the sintering temperature from 1005 to 920 °C. Besides, the obtained Ba(W_0.5Cu_0.5)O₃-doped ceramics sintered at 920 °C have optimized electrical properties, which are listed as follows: (K_p = 0.63, Q_m = 1415 and d₃₃ = 351 pC/N), and high depolarization temperature above 320 °C. These results indicated that this material was a promising candidate for high-power multilayer piezoelectric device applications.     

Effect of CuO on the sintering temperature and piezoelectric properties of MnO2-doped 0.75Pb(Zr0.47Ti0.53)O3-0.25Pb(Zn1/3Nb2/3)O3 ceramics

The sintering temperature of 0.75Pb(Zr_0.47Ti_0.53)O₃-0.25Pb(Zn_1/3Nb_2/3)O₃ ceramics containing 1.5 mol% MnO₂ was decreased from 930 to 850 °C with the addition of CuO. The CuO reacted with the PbO and formed a liquid phase during the sintering, which assisted the densification of the specimens. Most of the Cu²⁺ ions existed in the CuO second phase, thereby preventing any possible hardening effect from the Cu²⁺ ions. Variations of the k_p, Q_m, ?₃^T/?₀ and d₃₃ values with CuO were similar to that of the relative density. The specimen containing 0.5 mol% CuO sintered at 850 °C showed the good piezoelectric properties of k_p = 0.5, Q_m = 1000, ?₃^T/?₀ = 1750 and d₃₃ = 300 pC/N.     

Structure and electrical properties of MnO2-doped Sr2−xCaxNaNb5O15 lead-free piezoelectric ceramics

Lead-free piezoelectric ceramics Sr_2−xCa_xNaNb₅O₁₅ + y wt% MnO₂have been prepared by the conventional solid state reaction method. Our results reveal that Ca²⁺and Mn ions have entered into the Sr₂NaNb₅O₁₅ lattices to form a solid solution with tungsten-bronze structure. The substitution of Ca²⁺ induces a decrease in piezoelectric coefficient d₃₃, electromechanical coupling factors k_p and k_t, while, the addition of Mn ions decreases the sintering temperature and effectively promotes the densification of the ceramics. The effect of substitution of Ca²⁺and Mn ions on the structure, electrical properties and diffused phase changing were investigated systematically. For the ceramic with x = 0.05 and y = 0.5, the piezoelectric, dielectric and ferroelectric properties become optimum, giving a piezoelectric coefficient d₃₃ = 190 pC/N, electromechanical coupling factors k_p = 13.4% and k_t = 36.5%, ?_r = 2123, loss tangent tan δ = 0.038, remanent polarization P_r = 4.76 μC/cm², coercive field E_c = 12.68 kV/cm, and Curie temperature T_c = 260 °C.     

Preparation and electrical properties of perovskite ceramics in the system BaBi1−xSbxO3 (0 ≤ x ≤ 0.5)

The effect of the composition on the electrical properties of BaBi_1−xSb_xO₃ (0 ≤ x ≤ 0.5) negative temperature coefficient (NTC) thermistors was studied. Major phases present in the sintered bodies of BaBi_1−xSb_xO₃ (0 < x < 0.5) ceramics were BaBi_0.5Sb_0.5O₃ compounds with a rhombohedral structure and BaBiO₃ compounds with a monoclinal structure. Most pores were located in the grains of BaBiO₃ and BaBi_0.5Sb_0.5O₃ ceramics. It was apparent that the ρ₂₅ and B_25/85 constant of the thermistors increased with increasing Sb content.     

Phase transition and piezoelectric properties of K0.48Na0.52NbO3-LiTa0.5Nb0.5O3-NaNbO3 lead-free ceramics

Plate-like NaNbO₃ (NN) particles were used as the raw material to fabricate (1 − x)[0.93 K_0.48Na_0.52Nb O₃-0.07Li(Ta_0.5Nb_0.5)O₃]-xNaNbO₃ lead-free piezoelectric ceramics using a conventional ceramic process. The effects of NN on the crystal structure and piezoelectric properties of the ceramics were investigated. The results of X-ray diffraction suggest that the perovskite phase coexists with the K₃Li₂Nb₅O₁₅ phase, and the tilting of the oxygen octahedron is probably responsible for the evolution of the tungsten-bronze-typed K₃Li₂Nb₅O₁₅ phase. The Curie temperature (T_C) is shifted to lower temperature with increasing NN content. (1 − x)[0.93 K_0.48Na_0.52NbO₃-0.07Li(Ta_0.5Nb_0.5)O₃]-xNaNbO₃ ceramics show obvious dielectric relaxor characteristics for x > 0.03, and the relaxor behavior of ceramics is strengthened by increasing NN content. Both the electromechanical coupling factor (k_p) and the piezoelectric constant (d₃₃) decrease with increasing amounts of NN. 0.01-0.03 mol of plate-like NaNbO₃ in 0.93 K_0.48Na_0.52NbO₃-0.07Li(Ta_0.5Nb_0.5)O₃ gives the optimum content for preparing textured ceramics by the RTGG method.     

Coexistence of room temperature ferroelectricity and ferrimagnetism in multiferroic BiFeO3-Bi0.5Na0.5TiO3 solid solution

The structure, ferroelectric and magnetic properties of (1 − x)BiFeO₃-xBi_0.5Na_0.5TiO₃ (x = 0.37) solid solution fabricated by a sol-gel method have been investigated. X-ray diffraction and Raman spectroscopy measurements show a single-phase perovskite structure with no impurities identified. Compared with pure BiFeO₃, the coexistence of ferroelectricity and ferrimagnetism have been observed at room temperature for the solution with remnant polarization P_r = 1.41 μC/cm² and remnant magnetization M_r = 0.054 emu/g. Importantly, a magnetic transition from ferrimagnetic (FM) ordering to paramagnetic (PM) state is observed, with Curie temperature T_C ∼ 330 K, being explained in terms of the suppression of cycloid spin configuration by the structural distortion.     

Multiwavelength excited novel red-emitting phosphor Eu-activated Li2Zn2(MoO4)3

Eu³⁺-activated Li₂Zn₂(MoO₄)₃ multiwavelength excited red-emitting phosphors were synthesized via a solid state reaction. The structure and photoluminescence characteristics were investigated by X-ray powder diffraction and fluorescent spectrophotometry, respectively. The excitation spectrum included a strong broadband ranging from 250 to 350 nm and some sharp peaks at 363, 384, 395, 465, and 533 nm, which matchs the radiations of near-UV or blue light-emitting diodes chip well. Upon excitation either of near-UV or blue even green light, the intense red emission with 615 nm peak can be observed, which is ascribed to the ⁵D₀-⁷F₂ transition of Eu³⁺ ions. The chromaticity coordinates (x = 0.65, y = 0.34) of the as-obtained phosphor is very close to the National Television Standard Committee standard values (x = 0.67, y = 0.33). All these characteristics suggest that Eu³⁺-doped Li₂Zn₂(MoO₄)₃ wavelength-conversion material to be suitable candidate red component for phosphor-converted white light-emitting diodes.     

Ac electrical properties and dielectric relaxation of the new mixed crystal (Na0.8Ag0.2)2PbP2O7

The effect of Mn substitution on transport and thermoelectric properties of Cr_1?xMn_xSb₂ (x = 0, 0.01, 0.03, 0.05) have been investigated at the temperatures from 7 K to 313 K. The results show that similar to CrSb₂ all the doped samples are semiconducting. However, electrical resistivity of Cr_1?xMn_xSb₂ is found to decrease greatly with increasing doping content of Mn. Besides, Mn substitution leads to suppression of the plateau appearing in the plot of resistivity vs. temperature for CrSb₂ and makes the resistivity anomaly originating from antiferromagnetic transition shift to higher temperatures. Moreover, corresponding to the plateau a large peak of thermopower (?431 μV K^?1) was observed at ～60 K, which was also found to be suppressed by Mn doping. In addition, lattice thermal conductivity of Cr_1?xMn_xSb₂ was found to decrease substantially with increasing Mn content, though Mn doping also results in slow reduction in absolute value of thermopower at the temperatures T > ～200 K. As a result, at T > ～260 K the figure of merit ZT of heavily doped sample Cr_1?xMn_xSb₂ (x = 0.03 and 0.05) was improved. Specifically, at 313 K ZT value of Cr_0.95Mn_0.05Sb₂ is ～14% larger than that of CrSb₂, indicating that thermoelectric properties of CrSb₂ can be improved by proper substitution of Mn for Cr.