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1.
In this study, we investigated (1-x)Ba(Zr0.2Ti0.8)O3x(Ba0.7Ca0.3)TiO3 lead-free piezoelectric ceramics for energy harvester applications. The (1-x)BZT-xBCT ceramic is a promising lead-free piezoelectric material in the field of piezoelectric energy harvesting. Piezoelectric and energy properties of (1-x)BZT-xBCT ceramics were analyzed to confirm the possibility of using them as energy-harvesting materials. Especially, the vicinity of the phase convergence region was investigated to improve their piezoelectric properties. In the phase convergence region, cubic, rhombohedral, orthorhombic, and tetragonal regions co-exist within the narrow region. Near the phase transition region between the orthorhombic and tetragonal phase, the highest piezoelectric property d33?=?464 pC/N and the highest energy density of 158.5 μJ/cm3 were observed. This output energy density of 158.5 μJ/cm3 is the recorded highest value among lead-free ceramics. We found that the optimal sintering temperature was 1475?°C and the optimal composition was BZT-0.5BCT.  相似文献   

2.
《Ceramics International》2020,46(12):20284-20290
Lead-free (1-x)Ba(Ti0.8Zr0.2)O3-x(Ba0.7Ca0.3)TiO3 (BZT-BCT) possesses comparable piezoelectric constant with lead zirconate titanate (PZT), but its poor temperature electric performances stability and low Curie temperature limit its application. Here we designed composition graded BZT-BCT films with improved temperature stability of piezoelectric, ferroelectric, and dielectric performances over a wide temperature range, and the d33 reaches 21 pm/V with hysteresis loop even at 180 °C, which is far above the Curie temperature of BZT-BCT ceramic and BZT-0.5BCT film. The excellent temperature stability is ascribed to the lattice distortion and strain gradient in the grains caused by ions diffusion, and could suppress phase transition. This work could bring forward a feasible design for dielectric/piezoelectric/ferroelectric devices operating in harsh temperature environment.  相似文献   

3.
Good thermal stability in lead-free BaTiO3 ceramics is important for their applications above room temperature. In this study, thermal stable piezoelectricity in lead-free (Ba,Ca)(Ti,Zr)O3 ceramics was enhanced by tailoring their phase transition behaviors. Comparison between (1-x)Ba(Ti0.8Zr0.2)O3-x(Ba0.65Ca0.35)TiO3 and (1-y)Ba(Ti0.8Zr0.2)O3-y(Ba0.95Ca0.05)TiO3 revealed that latter system at y?=?0.80 had much better thermal stable piezoelectric coefficient than the former at x?=?0.45. Both systems crystalized in tetragonal to orthorhombic phase boundary at room temperature. The phase transition temperature and degree of diffusion were adjusted by Ca and Zr ions contents and demonstrated great influence on temperature dependent dielectric permittivity, hysteresis loops, and in-situ domain structures. The improved thermal stability of (1-y)Ba(Ti0.8Zr0.2)O3-y(Ba0.95Ca0.05)TiO3 prepared at y?=?0.80 was linked to its higher paraelectric to ferroelectric phase transition temperature (Tm?=?115.7?°C) and less degree of diffusion (degree of diffusion constant γ?=?1.35). By comparison, (1-x)Ba(Ti0.8Zr0.2)O3-x(Ba0.65Ca0.35)TiO3 prepared at x?=?0.45 revealed Tm?=?81.3?°C and γ?=?1.65. Overall, these findings look promising for future stimulation of phase transition behaviors and design of piezoelectric materials with good thermal stabilities.  相似文献   

4.
This work reports the composition dependent microstructure, dielectric, ferroelectric and energy storage properties, and the phase transitions sequence of lead free xBa(Zr0.2Ti0.8)O3-(1-x)(Ba0.7Ca0.3)TiO3 [xBZT-(1-x)BCT] ceramics, with x?=?0.4, 0.5 and 0.6, prepared by solid state reaction method. The XRD and Raman scattering results confirm the coexistence of rhombohedral and tetragonal phases at room temperature (RT). The temperature dependence of Raman scattering spectra, dielectric permittivity and polarization points a first phase transition from ferroelectric rhombohedral phase to ferroelectric tetragonal phase at a temperature (TR-T) of 40?°C and a second phase transition from ferroelectric tetragonal phase - paraelectric pseudocubic phase at a temperature (TT-C) of 110?°C. The dielectric analysis suggests that the phase transition at TT-C is of diffusive type and the BZT-BCT ceramics are a relaxor type ferroelectric materials. The composition induced variation in the temperature dependence of dielectric losses was correlated with full width half maxima (FWHM) of A1, E(LO) Raman mode. The saturation polarization (Ps) ≈8.3?μC/cm2 and coercive fields ≈2.9?kV/cm were found to be optimum at composition x?=?0.6 and is attributed to grain size effect. It is also shown that BZT-BCT ceramics exhibit a fatigue free response up to 105 cycles. The effect of a.c. electric field amplitude and temperature on energy storage density and storage efficiency is also discussed. The presence of high TT-C (110?°C), a high dielectric constant (εr ≈?12,285) with low dielectric loss (0.03), good polarization (Ps ≈?8.3?μC/cm2) and large recoverable energy density (W?=?121?mJ/cm3) with an energy storage efficiency (η) of 70% at an electric field of 25?kV/cm in 0.6BZT-0.4BCT ceramics make them suitable candidates for energy storage capacitor applications.  相似文献   

5.
《Ceramics International》2017,43(8):6175-6179
The xBi(Zn1/2Ti1/2)O3-BaTiO3 (xBZT-BT) ceramics, where x (mol) =0, 0.03, 0.06, 0.09, and 0.12, have been prepared by a solid-state reaction method. The phase transition, microstructure and optical properties were investigated. X-ray diffraction patterns indicate that the as-prepared samples have a polycrystalline perovskite structure. For x<0.06, the xBZT-BT ceramics exhibit clear tetragonal symmetry, and transform to rhombohedral phase as 0.06< x≤0.12. Coexistence of both tetragonal phase and rhombohedral phase is observed for x=0.06. The lattice strain is estimated by the Williamson-Hall analysis model, which suggests that the incorporation of substitution ions into the host lattice produces the inner stress field gives rise to structure distortions. The Raman scattering spectra corroborate the decrease in tetragonality with increasing the x, where the characteristic variation of phonon modes indirectly reveal the incorporation of Bi(Zn1/2Ti1/2)O3. Furthermore, the optical band gaps of xBZT-BT ceramics show a non-linear change, which can be explained by the crystal field theory and phase structure effect.  相似文献   

6.
Novel ((Bi0.5Na0.5)0.94Ba0.06)1-x(K0.5Nd0.5)xTiO3(x = 0.0, 0.02, 0.04, 0.06) lead-free ceramics (BNBT–xKN) were prepared by the solid-state reaction method. The effects of A-site (K0.5Nd0.5)2+ complex-ion substitution on their phase structure, dielectric, piezoelectric, and electromechanical properties were studied. The X-ray diffraction results indicate that all compositions are located in the morphotropic phase boundary (MPB) region where the tetragonal phase coexists with the rhombohedral phase. In addition, as the KN content increases, the ferroelectric order transform to relaxor order, which is characterized by a degeneration of maximum polarization, remnant polarization and correspondingly adjusts the ferroelectric-relaxor transformation temperature (TF-R) to room temperature. Interestingly, the disruption of ferroelectric phase caused a significant improvement of strains. A maximum strain of ~ 0.52% corresponding to normalized strain of ~ 612 pm/V appeared at 85 kv/cm for the x = 0.04 composition. Particularly, the composition of x = 0.04 exhibited high electrostrains of temperature insensitivity, which remained above 0.4% and kept within 10% from ambient temperature up to 110 °C. It can be ascribed to the coexistence of non-ergodic and ergodic states in the relaxor region. As a result, the systematic investigations on the BNBT–xKN ceramics can benefit the developments of temperature-insensitive “on-off” actuators.  相似文献   

7.
Ferroelectric ceramics in specific composition of 0.95Pb(ZrxTi1?x)O3–0.05Pb(Mn1/3Nb2/3)O3 or PZT–PMnN (with x=0.46, 0.48, 0.50, 0.52, and 0.54) have been investigated in order to identify the morphotropic phase boundary (MPB) composition. The effects of Zr/Ti ratio on phase formation, dielectric and ferroelectric properties of the specimens have also been investigated and discussed. X-ray diffraction patterns indicate that the MPB of the tetragonal and rhombohedral phase lies in x=0.52. The crystal structure of PZT–PMnN appeared to change gradually from tetragonal to rhombohedral phase with increasing Zr content. The dielectric and ferroelectric properties measurements also show a maximum value (εr, tan δ and Pr) at Zr/Ti=52/48, while the transition temperature decreases with increasing Zr content.  相似文献   

8.
《Ceramics International》2022,48(13):18452-18459
Bi0.5Na0.5TiO3 (BNT)-based dielectric ceramics have received a lot of attention due to the increased demand for pulse ceramic capacitors. However, comprehensive study on the relationship between their internal phase structure, dielectric characteristics, and ferroelectric properties is still lacking. The phase evolution and its impact on dielectric and ferroelectric properties of an important BNT-based solid solution, Bi0.5Na0.4K0.1TiO3-xSrTiO3 (x = 0, 0.1, 0.2, 0.3 and 0.4), were investigated systematically in this work using structural, dielectric, and ferroelectric characterization techniques. X-ray diffraction indicated the coexistence of rhombohedral and tetragonal phases. The frequency- and temperature-dielectric characterization was then used to derive the characteristic temperatures TB, Tm, Ts, and Td, and a phase diagram was developed. Furthermore, the temperature-dependent current against electric field curves and polarization versus electric field loops were used to derive the characteristic temperatures connected to high electric field features. This study not only explains the phase evolution of the Bi0.5Na0.4K0.1TiO3-xSrTiO3 solid solution, but it also correlates microscopic domains and polar nanoregions to macroscopic dielectric and ferroelectric properties.  相似文献   

9.
The crystal structure, domain patterns, and ferroelectric properties of Fe-modified BNT-ST [0.77(Bi0.5Na0.5)TiO3-0.23Sr(Ti1-xFex)O3] ceramics, fabricated by a conventional solid-state reaction, were investigated. Core-shell structures were observed and the volume fractions of the core-domain and shell (relaxor-matrix) were found to be dependent on Fe-modification content. The crystal structures of the core-domain and the relaxor-matrix were rhombohedral with the space group R3c, and the tetragonal with the space group P4bm, respectively. Compositional inhomogeneity, specifically, the enrichment of Bi3+ and Na+ and the considerable depletion of Sr2+, were observed in the core-domain region, and was reduced by substituting Ti4+ with Fe3+. The Fe-modification of the BNT-23ST ceramics promoted the diffusion of Sr2+ ions into the core region and shifted ferroelectric behaviour towards ergodic-relaxor behaviour. This improved the effective d33* of BNT-23ST ceramics to over 500 pm/V at 2 kV/mm.  相似文献   

10.
《Ceramics International》2020,46(6):7198-7203
To investigate the effect of Sm doping on the electrical properties of Ba(Zr0.2Ti0.8)O3-x(Ba0.7Ca0.3)TiO3 (BZT-xBCT) (x = 40, 50, 60) ceramics, three Sm-modified ceramics were prepared using the conventional solid-state reaction method. Related electrical measurements, including ferroelectric and dielectric investigations and impedance spectroscopy, were recorded for these ceramics. It was found that a tilted morphotropic phase boundary resulted from the addition of Sm, which induced the best piezoelectric properties and insulating behaviour in the Sm-BZT-60BCT sample. An abnormal P-E loop shrinkage appeared in the Sm-BZT-50BCT sample but not in the other two samples. This could be attributable to the different electronegativities between Ca2+ and Ba2+ and between Zr4+ and Ti4+, whose contents are different in varied samples and have an effect on defect-dipole alignment as well as spontaneous polarization. The activation energies for the bulk conductivity in the three composites were calculated to be 0.28 ± 0.01, 0.08 ± 0.01, and 0.36 ± 0.01 eV, confirming the existence of oxygen vacancies in our samples. The Sm dopant is responsible for the oxygen vacancies. This also leads to an increased Curie temperature in the three composites.  相似文献   

11.
In the present work, lead-free (Ba1?xCax)(Zr0.04Ti0.96)O3 (x=0.00–0.09) ceramics were fabricated via a solid-state reaction method. The microstructure and electrical properties of the ceramics were investigated. The microstructure of the BCZT ceramics showed a core shell structure at compositions of x=0.03 and 0.06. The substitution of small amount of Ba2+ by Ca2+ resulted in an improvement of the piezoelectric, dielectric and ferroelectric properties of the ceramics. The orthorhombic–tetragonal phase transition was found in the composition of x≤0.03. Piezoelectric coefficient of d33~392 pC/N and lowest Ec~3.3 kV/cm with highest Pr~14.1 μC/cm2 were obtained for the composition of x=0.03 while its Curie temperature (TC) was as high as 125 °C. However, the ferroelectric to paraelectric transition temperature had slightly shifted towards room temperature with increasing Ca2+ concentration.  相似文献   

12.
The crystal structure and dielectric properties of Ti4+-substituted CaSnSiO5 ceramic were investigated. Ti4+ entirely substituted Sn4+ of CaSnSiO5, and the solid solutions were formed at Ca(Sn1-xTix)SiO5 (0 ≤ x ≤ 1.0) ceramics. The evolutions of crystal structure were analysed through Rietveld refinement and transmission electron microscopy, and the phase transition from A2/a to P21/a space groups at Ca(Sn1-xTix)SiO5 (0.9 ≤ x ≤ 1.0) ceramics was clarified. The change in dielectric properties was related to the structural evolution of Ca(Sn1-xTix)SiO5 (0 ≤ x ≤ 1.0). The τf values of Ca(Sn1-xTix)SiO5 (0 ≤ x ≤ 0.4) ceramics initially decreased to +49.8 ppm/°C and then increased to +98.3 ppm/°C because of Sn/TiO6 octahedral distortion. The temperature coefficient of capacitance and εr anomaly peak were controlled by Ti4+ substitution for Sn4+ at Ca(Sn1-xTix)SiO5 (0.4 ≤ x ≤ 1.0) ceramics. The results provided a way to control the τf value of microwave dielectric ceramics.  相似文献   

13.
Solid solution ceramics of (1-x)Sr0.75Ba0.25Nb2O6-xPbZr0.52Ti0.48O3 (x = 0?0.4) were prepared and investigated. The phase evolves from tungsten bronze for x = 0, coexisted tungsten bronze and pyrochlore at x = 0.3, to pyrochlore for x> 0.3. As the results, the ceramics show dramatically composition dependent microstructure and electrical property. The grain shape changes from anisotropic pillar-like with maximum length-diameter ratio of 3.3 at x = 0.2 to isotropic cubic-like for x> 0.2. At the same time, the maximum dielectric constant temperature tends to decrease with an exceptional increase at x = 0.3 due to the coexisted phases. Interestingly, the x = 0.3 ceramic endures ultrahigh breakdown strength of 340 kV/cm, which, together with enhanced polarization, results in maximum recoverable energy storage density of 3.0 J/cm3and energy storage efficiency of 81.5 % at room temperature.  相似文献   

14.
《Ceramics International》2019,45(12):14768-14774
Ceramics of seven quasi-binary concentration sections of the ternary solid solution system (1-x-y)BiFeO3-xPbFe0.5Nb0.5O3-yPbTiO3 were prepared by the conventional solid-phase reaction method in the range of 0.05 ≤ x ≤ 0.325; 0.05 ≤ y ≤ 0.325. By using x-ray diffraction technique, the phase diagram of the system was constructed which was shown to contain the regions of tetragonal and rhombohedral symmetry and the morphotropic phase boundary between them. Grain morphology, dielectric and piezoelectric properties of selected solid solutions were investigated. The highest piezoelectric coefficient d33 = 50 pC/N was obtained. Dielectric characteristics of ceramics revealed ferroelectric relaxor behavior and region of diffuse phase transition from the paraelectric to ferroelectric phase in the temperature range of 600–800 K.  相似文献   

15.
《Ceramics International》2022,48(12):16956-16966
The Ba1-xLaxTi0.9Sn0.1O3 ceramics (x = 0, 0.006, 0.007, 0.008) were prepared by the traditional solid-state reaction method. The influence of La3+ on the phase, dielectric properties, ferroelectric properties, and electrocaloric effect (ECE) was analyzed in detail. The results of refinement show that all ceramics are multiphase coexistence at room temperature, including the cubic phase, the tetragonal phase, and the orthogonal phase. With the increase of La3+, the polar phases decrease but the non-polar phase increases, which is the main reason for the decline in adiabatic temperature change (ΔT). The analysis of dielectric properties and ferroelectric properties demonstrate that the diffuse phase transition is strengthened by introducing La3+. It also means that polar nanoregions (PNRs) might be formed. Therefore, the temperature stability of the Ba1-xLaxTi0.9Sn0.1O3 ceramics in a wide temperature range near room temperature is improved. Simultaneously, the PNRs provide additional entropy to improve ECE. A higher ΔT = 0.88 K is obtained under 60 kV/cm for x = 0.007, which also possesses excellent temperature stability in the temperature range of 298 K–378 K. The doping of La3+ also improves the electric field threshold of the electrocaloric strength (ΔTmax/ΔE) and stabilizes the ΔTmax/ΔE under a higher electric field, which is conducive to improving ECE under a higher electric field and providing another possible solution for promoting the practical application of ECE.  相似文献   

16.
Lead-free piezoelectric ceramics of Ba0.70Ca0.30Ti1?xFexO3 (x=0–0.03) have been synthesized by a conventional solid state reaction method. The influence of Fe content on the microstructure, phase transition, dielectric, ferroelectric, and piezoelectric properties is investigated systematically. The ceramics with x≤0.02 are diphasic composites of tetragonal Ba0.80Ca0.20TiO3:Fe and orthorhombic Ba0.07Ca0.93TiO3:Fe solid solutions. The tetragonal phase is gradually suppressed as x increases, the ceramic with x=0.03 is found to have diphasic pseudocubic and orthorhombic phases. And the grain size is dependent on Fe content significantly. Introduction of Fe at B-sites improves the densification and decreases the sintering temperature. As x increases from 0 to 0.03, the room temperature relative dielectric permittivity enhances, dielectric loss decreases, and the Curie temperature decreases monotonically from 128 °C to 58 °C. However, the ferroelectricity enhances slightly and reaches the maximum near x=0.005, and then weakens with increasing x. On the other hand, the piezoelectric coefficient (d33) and the electromechanical coupling coefficient (kp) decrease simultaneously with increasing x, whereas the mechanical quality factor (Qm) increases significantly. The structure–electrical properties relationship is discussed intensively to give more information on (Ba,Ca)TiO3-based lead-free piezoelectric ceramics.  相似文献   

17.
The ternary (1?x)(0.8BiFeO3-0.2BaTiO3)-xK0.5Na0.5NbO3 (0?≤?x?≤?0.5) solid solutions have been successfully synthesized by a solid-state reaction route. X-ray diffraction and Rietveld refinement studies reveal the phase transition from the rhombohedral and tetragonal phases to the single tetragonal phase with x increasing. The average grain size decreases initially and then increases as x increases, whereas the remnant magnetization shows an opposite trend and reaches the maximum value of ~2.09?emu/g at x?=?0.3. An enhanced remnant polarization of ~8.6?μC/cm2 appears at x?=?0.3 due to the structure distortion and the decrement of defects. Moreover, the remanent polarization and the relative permittivity reach the maximum value of ~20.14 μC/cm2 (10?Hz) and ~644 (1?kHz) at x?=?0.5, respectively, and the corresponding dielectric loss decreases to the lowest value of ~0.022 (1?kHz). These results indicate that the properties of ternary BFO-BTO-KNN solid solutions can be modulated by adjusting the K0.5Na0.5NbO3 content to adapt to different application needs.  相似文献   

18.
We report on the correlation between structural, ferroelectric, piezoelectric and dielectric properties of the (1-x)Ba0.7Ca0.3TiO3-xBaTi0.8Zr0.2O3 (x?=?0.45, 0.55; abbreviated as 55BCT30 and 45BCT30) ceramics close to morphotropic phase boundary (MPB) region. The 55BCT30 and 45BCT30 ceramics were synthesized by the standard, high-temperature solid state ceramic method. X-ray diffraction (XRD) along with Rietveld refinement indicate that the 55BCT30 ceramics exhibit rhombohedral (R, space group R3m), orthorhombic (O, space group Amm2) and tetragonal (T, space group P4mm) phases while 45BCT30 ceramics exhibit only T and O phases. The temperature dependent Raman spectroscopy measurements confirm the structure and phase transformations observed from XRD. All the ceramics are chemically homogeneous and exhibit a dense microstructure with a grain size of 5–7?µm. The presence of polarization-electric field and strain-electric field hysteresis loops confirm the ferroelectric and piezoelectric nature of the ceramics. The polarization current density-electric field curves show the presence of two sharp peaks in opposite directions indicating the presence of two stable states with opposite polarity. Higher values of direct piezoelectric coefficient (d33 ~?360 pC/N) were observed due to the existence of low energy barrier near MPB region and polymorphism. The 55BCT30 ceramics exhibit a higher value of electrostrictive coefficient (Q33 ~?0.1339?m4/C2) compared to the well-known lead-based materials. The temperature dependent dielectric measurements indicate the O to T phase transition for 55BCT30 and 45BCT30. These ceramics exhibit a Curie temperature (Tc) of 380?K with a dielectric maximum of ~ 4500.  相似文献   

19.
(Pb0.97Ba0.02)Nb0.02(Zr0.55Sn0.45?xTix)0.98O3 (PBNZST, 0.03≤x≤0.06) ceramics were prepared by conventional solid state synthesis and their crystal structure, ferroelectric, dielectric, and electric field-induced strain properties were systemically investigated. A transformation from antiferroelectric (AFE) phase to ferroelectric (FE) phase was observed at 0.05<x<0.06. Besides, with the increase of Ti content, the electric field-induced strain decreased, due to the larger strain of AFE ceramics compared to FE ceramics. Further, when the measuring frequency decreased, the strain improved, because the electric field at low frequency allows a more efficient switching of domains, resulting in larger strain. The maximum strain of 0.55% was obtained in (Pb0.97Ba0.02)Nb0.02(Zr0.55Sn0.45?xTix)0.98O3 antiferroelectric ceramics with x=0.03 at 2 Hz.  相似文献   

20.
《Ceramics International》2020,46(3):3257-3263
0.6(Na0.5Bi0.5)TiO3-0.4(Bi1-ySry)TiO3 ceramics (abbreviated BNT-BSyT, y = 0.2, 0.3, 0.5, 0.7, and 0.9 mol) were fabricated using a traditional solid-state processing route, and the effects of Sr2+ on phase structure, di- and ferroelectric properties, and electrostrictive properties were systematically investigated. The values of γ for BNT-BSyT ceramics are greater than 1.8, revealing that these materials exhibit relaxor ferroelectric properties derived from the co-occupation of Bi3+, Na+, and Sr2+ in the A-site and inhomogeneous polarization states (i.e., coexistence of rhombohedral and tetragonal states). In addition, Td decreases with increasing Sr2+ content along with a stable and increased tetragonal phase. BNT-BS0.9T ceramic has a slightly large maximum polarization Pmax = 16.15 μC/cm2, a small remanent polarization Pr = 1.6 μC/cm2, and a relatively good energy storage property (density W1 = 0.220 J/cm3 and efficiency η = 72.13%), indicating that Sr2+ substitution helps to promote energy storage characteristics. Moreover, there is a superior electrostrictive coefficient (Q33 = 0.0385 m4/C2) for BNT-BS0.3T ceramic. Therefore, we propose that this lead-free electrostrictor is a good candidate for practical applications.  相似文献   

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