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Lead-free piezoceramics based on the (Ba, Ca)(Zr, Ti)O3 (BCZT) system exhibit excellent electromechanical properties for low-temperature actuation applications, but suffer from relatively high processing temperatures. Here we demonstrate an approach for the reduction of the sintering temperature and simultaneous increase of the electromechanical strain response of (Ba, Ca)(Zr, Ti)O3 piezoceramics by aliovalent doping with Ce. The samples were prepared by solid state synthesis and their crystallographic structure, dielectric, ferroelectric, and electromechanical properties were investigated. The highest d*33 value of 1189 pm/V was obtained for the sample with 0.05 mol% Ce, substituted on the A-site of the perovskite lattice. The results indicate a large potential of these materials for off-resonance piezoelectric actuators.

When employed appropriately, ferroelectric materials present themselves as one of the most efficient means of waste (thermal/mechanical) energy scavenging. A large conversion potential can be obtained when appropriate materials are combined with high-field actuation (Ericsson cycle). However, waste energy rarely presents itself in an isolated form (heat or vibration). There is also a distinct lack of systems capable of simultaneous thermomechanical energy conversion, especially in the low-frequency range. In this regard a systematic approach to the concept of combined energy harvesting and storage potential of a singular material system is presented. Polarization versus electric field hysteresis loops were gathered as a function of temperature, uniaxial compressive stress, and electric field. Thereafter, a theoretical assessment was made to the effect of the biased and unbiased energy conversion potential of 0.50Ba(Zr0.2Ti0.8)O3– 0.50(Ba0.7Ca0.3)TiO3 bulk lead-free ferroelectric material. Maximum energy conversion potentials of 150 and 210 kJm@3 were obtained for thermal (5 MPa, 24–96 8C) and mechanical cycles (24 8C, 5–160 MPa), respectively. A slightly improved performance of 220 kJm@3 was obtained under simultaneous depolarization, despite performance degradation through individual biasing. However, the energy-storage density improved by 100% (80 kJm@3) and 50% (60 kJm@3), respectively, when operated under elevated stress (60 MPa) and temperature (90 8C). Results are indicative of a singular material system that could be used for combined thermomechanical energy conversion and on-board storage capacity.

© 2017 The American Ceramic Society Surface chemistry and topo-physical properties determine the interactions of biomaterials with their physiological environment. Ferroelectrics hold great promise as the next generation of scaffolds for tissue repair since they feature tunable surface electrical charges, piezoelectricity, and sensing capabilities. We investigate the topography, wettability, chemical stability, and cytotoxicity in salient ferroelectric systems such as (1−x) (Na1/2Bi1/2)TiO3–xBaTiO3, (1−x)Ba(Zr0.2Ti0.8)O3−x(Ba0.7Ca0.3)TiO3, and Pb(Zr,Ti)O3 to test their suitability as biomaterials. The lead-free ferroelectrics promote in vitro cell viability and proliferation to a considerably high extent. 0.94 mol % (Na1/2Bi1/2)TiO3–0.06 mol% BaTiO3 showed the greatest potential leading to a cell viability of (149 ± 30)% and DNA synthesis of (299 ± 85)% in comparison to the reference. Lead leaching from Pb(Zr,Ti)O3 negatively affected the cultured cells. Wettability and chemical stability are key factors that determine the cytotoxicity of ferroelectrics. These variables have to be considered in the design of novel electroactive scaffolds based on ferroelectric ceramics.

Lead-free Ba(Zr0.2Ti0.8)O3-0.5(Ba0.7Ca0.3)TiO3 (BZT-0.5BCT) ceramics have drawn attention in recent years because of their outstanding dielectric and electromechanical properties, such as a piezoelectric coefficient d33 ∼ 620 pC N−1 and a large signal of d 33 * ∼ 1100 pm V−1 at 0.5 kV mm−1 at room temperature (RT). These particular properties are relevant to a range of applications. However, the structural origin of this high piezoelectric coefficient is still a subject of discussion. An in-depth understanding of the ferroelectric domain evolution of BZT-0.5BCT ceramics is crucial for probing the underlying mechanisms and for guiding practical applications. Using piezoresponse force microscopy (PFM), we have directly visualized the evolution of the BZT-0.5BCT domain structure using temperature and electric field stimulation on micrometer and nanometer scales. The PFM results unambiguously evidence the coexistence of wedge-shaped and lamellar domains with miniaturized nanodomain structures at RT. The temperature- and electric-field-dependent PFM study presented here highlights the critical role of wedge-shaped domains in domain evolution. Wedge-shaped domains turn into small domains with curved domain walls after the heating cycle and then become lamellar domains after the poling cycle at RT. Transitional domain structures with an increased density of nanodomains appear in both the thermal and poling cycles. More interestingly, the electric-field-dependent domain structure evolution at different temperatures shows better domain structure reversibility at high temperatures than at temperatures close to the phase boundary. This demonstrates that the BZT-0.5BCT ceramic has superior stability at medium temperatures (40 °C–60 °C), implying excellent stability for applications.

Lead-free Ba0.85Ca0.15Zr0.1Ti0.9O3 (BCZT) piezoceramics with Bi2O3 additive were synthesized using solid-state ceramic processing. Various amounts of Bi2O3 (0.05, 0.1, 0.5, and 1.0 mol%) were added after calcination, milled, compacted, and sintered with no compensation at A- or B-sites. Addition of up to 0.5 mol% Bi2O3 was found to greatly enhance the densification and increase the piezoelectric properties, while higher amounts decreased the grain size and induced relaxor-like electrical behavior, obeying the Vogel-Fulcher model. The highest properties were obtained for the BCZT with 0.1 mol% Bi2O3 sintered at 1350 °C: d33 = 325 pC/m, d33* = 509 pm/V (at 3 kV/mm), kp = 0.42, and Pr = 10.4 μC/cm2. The microstructure, phase composition, and local structure were investigated by scanning electron microscopy, X-ray diffraction, and Raman spectroscopy. The appearance of the A1g vibration mode in the Raman spectra and the shift of diffraction peaks to lower 2θ values indicate the incorporation of Bi3+ into the B-site of the perovskite BCZT structure.

The Bi1/2Na1/2TiO3-based materials exhibit the largest electric-field-induced strains among lead-free piezoceramics and are considered as promising candidates for actuation applications. A typical representative of this group is (1-x)Bi1/2Na1/2TiO3-xSrTiO3, where its excellent electromechanical properties were recently related to the existence of a core–shell microstructure. Although the latter was also reported in other Bi1/2Na1/2TiO3-based ceramics, the formation mechanism remains unknown. In the present work we therefore first investigated the solid-state reaction occurring during calcination using simultaneous thermogravimetric analysis, X-ray diffraction, scanning and transmission electron microscopy. The reaction occurred in two steps, whereby the cores and shells had different formation reaction temperatures, which resulted in a metastable heterogeneous microstructure. Furthermore, a series of sintered samples with different relative densities, grain sizes, and core densities was prepared. Modifications of these microstructural parameters resulted in variation of the maximal strain by 17% and in the electric-field required to trigger the phase transitions by 38%.

The affiliation of author “Raziye HAYATI” in the original version of this article was unfortunately wrongly written on page 186, instead of Semiconductor Division, Materials and Energy Research Center, Karaj 31787/316, Iran It should read Department of Materials Engineering, Yasouj University, Yasouj, 75918-74934, Iran

© 2017 The American Ceramic Society The lead-free (1−x)Ba(Zr0.2Ti0.8)O3-x(Ba0.7Ca0.3)TiO3 system is considered as promising candidate for the replacement of lead-based piezoceramics in actuation applications, during which electric fatigue is a major concern. This issue was addressed in this work, where the unipolar fatigue resistance of three (1−x)Ba(Zr0.2Ti0.8)O3-x(Ba0.7Ca0.3)TiO3 compositions with different crystallographic structures (rhombohedral, orthorhombic, and tetragonal) was evaluated. Strain asymmetry and development of an internal bias field were observed in all compositions. The decrease in the remanent polarization and the large signal piezoelectric coefficient after 107 unipolar cycles was found to lie between 6%-12% and 2%-13%, respectively. The most pronounced fatigue was observed for the orthorhombic composition, which has the largest extrinsic contribution to strain. On the other hand, the best fatigue resistance was observed for the tetragonal composition, which has a predominantly intrinsic strain response. The correlation of fatigue resistance with strain mechanism was corroborated with determination of the Rayleigh parameters and changes in the domain morphology after cycling as confirmed by piezoresponse force microscopy.

The macroscopic electromechanical behavior of lead-free bilayer composites was characterized at room temperature. One layer consisted of a nonergodic relaxor, (Bi1/2Na1/2)TiO3–7BaTiO3, with an electric-field-induced longrange ferroelectric order, whereas the other is understood to be an ergodic relaxor [(Bi1/2Na1/2)TiO3–25SrTiO3] that undergoes a reversible electric-field-induced macroscopic nonpolar-to-polar transition. Microstructural evidence of a bilayer with low diffusion between the two components is also demonstrated. By taking advantage of the different macroscopic strain– and polarization–electric-field responses of the two constituents, internal mechanical and electrical fields can be developed that enhance the unipolar strain over that expected by a rule of mixtures approximation, thereby improving the properties needed for application of such materials to actuator systems. It is possible through further tailoring of the volume fractions and macroscopic properties of the constituents to optimize the electromechanical properties of multilayer lead-free ferroelectrics.

We present a critical review that encompasses the fundamentals and state-of-the-art knowledge of barium titanate-based piezoelectrics. First, the essential crystallography, thermodynamic relations, and concepts necessary to understand piezoelectricity and ferroelectricity in barium titanate are discussed. Strategies to optimize piezoelectric properties through microstructure control and chemical modification are also introduced. Thereafter, we systematically review the synthesis, microstructure, and phase diagrams of barium titanate-based piezoelectrics and provide a detailed compilation of their functional and mechanical properties. The most salient materials treated include the (Ba,Ca)(Zr,Ti)O3, (Ba,Ca)(Sn,Ti)O3, and (Ba,Ca)(Hf,Ti)O3 solid solution systems. The technological relevance of barium titanate-based piezoelectrics is also discussed and some potential market indicators are outlined. Finally, perspectives on productive lines of future research and promising areas for the applications of these ma...

The influence of the uniaxial preload on the off-resonance actuation performance of piezoelectric ceramics was investigated for compressive preload values up to −80 MPa. The study was performed on soft-type lead zirconate titanate (PZT), being the most widely used piezoelectric material. The samples were analysed using the proportional loading method, which enables the simultaneous application of electrical and mechanical loads, thereby mimicking the real operation conditions over the full stress–strain range. An increase of the blocking stress and the longitudinal piezoelectric stress coefficient was observed for all the applied preload values. The optimum properties, a blocking stress of −56 MPa and a free strain of 0.23%, were obtained at a preload value of −40 MPa and electric field of 2 kV mm − 1. This represents an increase of 16% and 20%, respectively, as compared to the values obtained at the smallest preload. In addition, the maximum work output was increased by about 28%. Finally, the results obtained at the lowest preload of −4 MPa using the proportional loading method were compared to the operational ranges determined by other methods. The comparison revealed large discrepancies between the methods, originating from the different order of the application of electrical and mechanical fields and the inherent nonlinearity of ferroelectric materials. This discrepancy results in decreased actuator performance due to impedance mismatching, demonstrating the need for accurate determination of the actuator's operational range.